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2019

KUR16 Progress Report 201
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Published by
Institute for Integrated Radiation and Nuclear Science,
Kyoto University,
Kumatori-cho, Sennan-gun, Osaka 590-0494 Japan

It is a great pleasure for us to publish the KURNS Progress Report 2019. This report contains allof the accomplishments of research and related activities at Institute for Integrated Radiation and
Nuclear Science, Kyoto University (KURNS) during the fiscal year 2019 from April 2019 to March
2020. 㻌 Our institute continues to play a distinctive role as a Joint Usage/Research Center,promoting an extensive range of studies from fundamental to applied research with research
reactors and accelerators.
It is reassuring to note that the number of applications for Joint Research are still increasing
although the reactors had sustained operations for several years. We are proud since thisdemonstrates that researchers and students support our activity, which endorses our facilities as
indispensable tools in their research activities with quantum beam and radioisotope. In the pastfiscal year, KUR was operated for 849 hours and KUCA was for 774 hours. In total, we accepted
4,477 man-day researchers and students for using research facilities and for attending scientificmeetings. A large number of research subjects has been enrolled, which covers various fields ofnuclear science and technology, material science, radiation life science and radiation medical
science. We proudly announce that the clinical trial of the boron neutron capture therapy (BNCT)
has finished successfully, and it becomes a practical medical care after long-term basic researches
in KUR.
We strive for safe and stable operations for nationwide use, making it our primary mission toprovide scientists the opportunity to conduct research and education. We are happy to dedicate our
support to enable users conduct significant interdisciplinary research at KURNS.
Kumatori, June 8, 2020
Yuji Kawabata
Director, KURNSCONTENTS
I. ANNUAL SUMMARY OF EXPERIMENTAL RESEARCH ACTIVITIES ...............................

1

I-1. PROJECT RESEARCHES ...........................................................................................................

2

Project 1 Project Research on Nuclear Spectroscopy and Condensed Matter Physics Using Short-Lived
NucleiY. Ohkubo (31P1) ..................................................................................................................
PR1-1
Technique of Transferring Radioactive Atomic Nuclei Implanted in Dry Ice Film
A. Taniguchi et al. (31P1-1) ·········································································
PR1-2β-Decay Spectroscopic Studies of Fission Products Using a Clover Detector
Y. Ishikawa et al. (31P1-2) ··········································································
PR1-3
Linear Polarization Measurement for γ Rays from 148Pr
Y. Kojima et al. (31P1-3) ············································································
PR1-4
Measurement of the Internal Pressure in Ultrafine Bubbles by Angular Correlation Technique
M. Tanigaki et al. (31P1-5) ··········································································
PR1-5
Temperature-Dependent Polaronic Local Structures in La0.7Ca0.3MnO3 Observed through Spin
Relaxation of TDPAC Probe Nuclei
W. Sato et al. (31P1-6) ···············································································
PR1-6
Local Structure of In Impurities Doped in SrTiO3 Studied by TDPAC Method
S. Komatsuda et al. (31P1-7) ·······································································
Project 2 Project Research of Accelerator-Driven System with Spallation Neutrons at Kyoto University
Critical Assembly
C. H. Pyeon (31P2) ························································································
PR2-1
Subcriticality Monitoring for a Reactor System Driven by Spallation Source (III)K. Hashimoto et al. (31P2-1) ·······································································
PR2-2
Measurement of Reaction Rates of Intermediate Neutrons on Accelerator-Driven Systemwith Spallation Neutrons
N. Aizawa et al. (31P2-2) ············································································
PR2-3
Measurement of 243Am Fission Rates in Low-Enriched Uranium Region at A-core of KUCA
A. Oizumi et al. (31P2-3) ············································································
PR2-4
Development of Real-time Subcriticality Monitor
K. Watanabe et al. (31P2-5) ·········································································
Project 3 Preclinical Study for Development of New Drug for NCT
M. Suzuki (31P3) ··························································································
PR3-1
Screening of Boron Compound for BNCT International Collaboration Studies
M. Takagaki and M. Suzuki. (31P3-1) ·····························································PR3-2
The Self-assembling A6K Peptide Nanotube as BSH Delivery System
H. Michiue et al. (31P3-2) ············································································
PR3-3
Chemical Functionalization of Boron-Containing Nanoparticle and its Application to
Boron Neutron Capture Therapy
Y. Wang et al. (31P3-3) ··············································································
PR3-4
Examining Efficacy of Tumor Models for BNCTK. Matsumoto et al. (31P3-4) ·······································································
PR3-5
Development of New Boron Drug for Next-generation A-BNCT Treatment
S. Ishiyama et al. (31P3-7) ··········································································
PR3-6
Research and Development on Next-generation A-BNCT Treatment
S. Ishiyama et al. (31P3-8) ··········································································
PR3-7
Evaluation of Boron Neutron Capture Therapy (BNCT) Using Brain Tumor Bearing Ratsor Mice Model
Y. Fukuo et al. (31P3-11) ············································································
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PR3-8

PR3-9
PR3-10

PR3-11

PR3-12
PR3-13PR3-14
PR3-15
PR3-16
PR3-17
PR3-18Intracellular Target Delivery of Cell-penetrating Peptide-conjugated Dodecaborate for
Boron Neutron Capture Therapy (BNCT)I. Nakase et al. (31P3-12) ···········································································A Novel Carbon Nanohrns for BNCT
T. Tsurubuchi et al. (31P3-13) ······································································Development of a Multifunctional Nanoparticle towards Next-generation Boron Neutron
Capture Therapy
A. Kim et al. (31P3-14) ··············································································
Design, Synthesis, and Evaluation of Glucose and Macrocyclic Polyamine-type Boron
Carriers for BNCT
S. Aoki et al. (31P3-15) ··············································································
Boron Neutron Capture Therapy using Polymer-Based Boron Delivery Systems
T. Nomoto et al. (31P3-16) ··········································································Development of Carrier Protein-based Boron Delivery System
H. Nakamura et al. (31P3-17) ·······································································Development of Novel Boron Agents for BNCT against Malignant Brain Tumors
A. Fujimura et al. (31P3-18) ········································································
Experiment on the Anti-tumor Effect of Pegylated BSH by Thermal Neutron Irradiation
M. Shirakawa et al. (31P3-19) ······································································
Preparation and Characterization of BODIPY-Tethered Oligonucleotides for BNCTK. Tanabe et al. (31P3-20) ···········································································
In vivo Evaluation of BNCT for 5-FU Resistant Oral Squamous Cell Carcinoma
K. Igawa et al. (31P3-21) ············································································
Anti-tumor Evuluation of Gadolinium Neutron Capture Therapy through comparison ofTumor Size using Gd-DTPA-incorporated Calcium Phosphate Nanoparticles
H Xuan et al. (31P3-22) ·············································································

Project 4 Clinical Research on Explorations into New Application of BNCT
M. Suzuki and H.Yanagie. (31P4) ...........................................................................................
PR4-1
Clinical Research on Explorations into New Application of BNCT
M. Suzuki et al. (31P4-1) ············································································
PR4-2
Preparation of Boron entrapped WOW emulsion by Mixing Medical Device for Boron
Neutron Capture Therapy to Hepatocellular Carcinoma
H. Yanagie et al. (31P4-2) ................................................................................................
Project 5 Establishment of Integrated System for Dose Estimation in BNCTY. Sakurai (31P5) ··························································································
PR5-1

PR5-2
PR5-3
PR5-4
PR5-5

PR5-6
PR5-7

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Establishment of Characterization Estimation Method in BNCT Irradiation Field using
Bonner Sphere and Ionization Chamber (III)Y. Sakurai et al. (31P5-1) ············································································

42

Study on New Type of Neutron Spctrometer for BNCT
A. Uritani et al. (31P5-2) ············································································

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Neutron Measurement by using the Self-activation of Iodine-added Plastic Scintillators
A. Nohtomi et al. (31P5-4) ··········································································
Characterization of Active Neutron Detector for Boron Neutron Capture Therapy
M. Takada et al. (31P5-5) ············································································
Study for Microdosimetry using Silicon-on-insulator Microdosimeter in the BNCT
Irradiation Field (III)Y. Sakurai et al. (31P5-6) ············································································
Measurement of BNCT Beam Component Fluence with Polymer Gel Detector
K. Tanaka et al. (31P5-7) ············································································Development of Neutron Fluence Distribution Measuring Device using
Thermoluminescence Slabs
K. Shinsho et al. (31P5-8) ············································································
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PR5-8The Study for Development and Application of Tissue Equivalent Neutron Dosimeter
M. Oita et al. (31P5-9) ················································································

49

Development and Evaluation of 3D Gel Dosimeter for the Measurement of dose
Distribution in BNCTS. Hayashi et al. (31P5-10) ···········································································

50

Establishment of Beam-quality Estimation Method in BNCT Irradiation Field using Dual
Phantom Technique (III)Y. Sakurai et al. (31P5-11)·············································································

51

Characteristics test of a Prpmpt Gamma-ray detector using LaBr3(Ce) Scintillator
and 8 x 8 Array MPPC for Boron Neutron Capture Therapy
K. Okazaki et al. (31P5-12)···········································································

52

Development of Fiber-reading Radiation Monitoring System with a Red/Infrared-emitting Scintillator at 60Co Radiation Facilities
S. Kurosawa et al. (31P5-13) ·········································································

53

Establishment of the Imaging Technology of 478 keV Prompt Gamma-rays of
Boron-neutron Capture Reaction and the Measurement of the Intensity of the Neutron Field
T. Mizumoto et al. (31P5-14)·········································································

54

Feasibility Study of a Gel-dosimeter for a Quality Assurance and a Quality Control in
Boron Neutron Capture Therapy
S. Nakamura et al. (31P5-15)·········································································

55

Optimization of Bolus Shape for Boron Neutron Capture Therapy Using Epi-thermal
Neutron Beam
T. Takata et al. (31P5-16) ·············································································

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PR5-16Development of Novel Radiochromic Gels for Assesing 3-Dimensional dose Distributionin Brain
H. Yasuda et al. (31P5-17) ············································································

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PR5-17

Measurement of Neutron Distributions in the BNCT Irradiation Field using a GEM Detector
S. Uno et al. (31P5-18) ················································································ 58

PR5-18Development of Epi-thermal Neutron Flux Intensity Detector for BNCT
I. Murata et al. (31P5-20) ·············································································
Investigation of Thermal Neutron-Induced Soft Errors in Semiconductor Devices
H. Tanaka et al. (31P5-21) ············································································

PR5-9

PR5-10

PR5-11

PR5-12

PR5-13

PR5-14

PR5-15PR5-19Project 6 Analyzing Tumor Microenvironment and Exploiting its Characteristics in Search of
Optimizing Cancer Therapy Including Neutron Capture Therapy
S. Masunaga (31P6) ·······················································································

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PR6-1

Effect of a Change in Reactor Power on Response of Murine Solid Tumors in vivo, Especiallyon that of Quiescent Tumor Cells, in Boron Neutron Capture Therapy
S. Masunaga et al. (31P6-1)··········································································· 63

PR6-2

Development of New Amino Acid-type Boron Carriers for BNCT
A. Matsushita et al. (31P6-2) ·········································································

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PR6-3

Molecular Mechanism Underlying HISP2-mediated Radioresistance of Hypoxic Tumor Cells
M. Kobayashi et al. (31P6-3) ········································································· 65

PR6-4

OH Radicals from the Indirect Actions of Neutron Beam Induce Cell Killing
R. Hirayama et al. (31P6-4) ··········································································

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Intracellular Delivery of Membrane-fluidity Sensitive Boron Liposomes with
Tumor-specific Cell Penetrating Peptides
S. Kasaoka et al. (31P6-5) ············································································

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PR6-5

PR6-6

Preparation and Characterization of a Novel Bispecific Antibody That Targets Her2 and BSH for
Boron Neutron Capture Therapy
T. Kanai et al. (31P6-6) ··············································································· 68

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PR6-7Development of Novel BPA-Tirapazamine Hybrid BNCT Agent Targeting Hypoxic
Tumor Cells
Y. Uto et al. (31P6-7) ··················································································

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PR6-8

The Tumor Invasion Enhanced by the Conditioned-medium after X-irradiation
H. Yasui et al. (31P6-8)················································································

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Analysis of the Response of Tumor Tissue and Cells to BNCTS. Imamichi et al. (31P6-9) ···········································································

71

The Contribution of Blood Boron-neutron Reaction to Subcutaneous Tumor Growth
Suppression was Equal to that of Neutrons Irradiation Only GroupK. Nakai et al. (31P6-10) ·············································································

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Cell Killing Effect of BNCT with Novel Boron Compound SMA Glucosamine Complex
Y. Matsumoto et al. (31P6-11)········································································

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Attempts to Sensitize Tumor Cells by Exploiting the Tumor Microenvironment
Y. Sanada et al. (31P6-12) ············································································

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Project Research on Advances in Isotope-Specific Studies Using Muti-Element Mössbauer
Spectroscopy
M. Seto (31P8) ···························································································

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PR6-9
PR6-10

PR6-11
PR6-12

Project 8

PR8-1

PR8-2

PR8-3
PR8-4
PR8-5
PR8-6
PR8-7

PR8-8
PR8-9

Project 9

PR9-1
PR9-2
PR9-3

Analysis of Iron-based Products Using Mössbauer Spectroscopy- Iron Oxide Scale Generated in the Boiler Feed-water in Thermal Power Plant –Y. Akiyama et al. (31P8-1)············································································EFG Tensor of Fe2+ in M2 site of Orthopyroxene by Single Crystal
Mössbauer Microspectroscopy
K. Shinoda and Y. Kobayashi. (31P8-2)·····························································
Temperature Dependence of Mössbauer Spectra for Fe2O3-Al2O3 Solid Solution
S. Takai et al. (31P8-3) ················································································A Nuclear Resonance Vibrational Spectroscopic Study of Oxy Myoglobin
T. Ohta et al. (31P8-4) ·················································································
Mössbauer Spectroscopy on the Antiperovskite Oxide Superconductor Sr3−xSnO
Y. Maeno et al. (31P8-5) ··············································································
Researches on Magnetism in a Novel Kondo LatticeY. Kamihara et al. (31P8-6)···········································································
Study on Structure of Gold Complexes Coordinated with α-Amino Acids by Means of197
Au Mössbauer Spectroscopy
H. Murayama et al. (31P8-7) ·········································································
197
Au Mössbauer Study of Supported Au Nanoparticles Catalysis II
Y. Kobayashi et al. (31P8-8)··········································································Development of Mössbauer Spectroscopy for 166Er
S. Kitao et al. (31P8-9) ················································································
Project Research on Boron Dynamics in Plants using Neutron Capture Reaction: Developmentof Boron Analytical Method and Elucidation of its Physiological Function
T. Kinouchi (31P9) ······················································································
Analysis of Boron Transport within Roots Using Neutron Capture Radiography
M. Kobayashi and T. Kinouchi. (31P9-1) ···························································
Analysis of Localization of Boron in Root Tissues by Neutron Capture Radiography
S. Kitajima et al. (31P9-2) ············································································
Improvemnt of In Situ Visualization of Boron Distributed in Plants by Neutron Radiation
T. Kinouchi (31P9-3) ··················································································

Project 10 The Effect of Boron Neutron Capture Therapy on Normal Tissues
M. Suzuki (31P10) ·················································································
PR10-1The Effect of Boron Neutron Capture Therapy (BNCT) on Normal Lung in Mice
M. Suzuki and Y. Tamari. (31P10-1)·································································

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PR10-2
PR10-3

Study of the Influence on Normal Liver tissue by BNCTY. Tamari et al. (31P10-4)·············································································The Effect of Boron Neutron Capture Therapy to Normal Bones in MiceR. Iwasaki et al. (31P10-5) ···········································································

Project 11 Preclinical Studies on Gadolinium Neutron Capture Therapy
M. Suzuki (31P11) ························································································

PR11-1

PR11-2

Investigation of Cell Killing Effect by Auger Electrons Emitted during Gadolinium
Neutron Capture Therapy (Gd-NCT)
M. Suzuki and H. Tanaka (31P11-1) ·································································
Investigation of Gadolinium Neutron Capture Therapy (Gd-NCT) using
Gadolinium-loaded Nano-particle
M. Suzuki et al. (31P11-2) ············································································

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PR11-3

Nanoparticulate Formulations for Neutron Capture Therapy: Evaluation of Amti-tumor
Effect after Intratumor Injection
T. Andoh et al. (31P11-3) ············································································· 100

PR11-4

Examination on Gadolinium Neutron Capture Therapy in Mouse Malignant Melanoma
Bone Metastasis Model
T. Matsukawa et al. (31P11-4)········································································ 101

PR11-5Preparation of Drugs Bearing Hoechst unit that Target Cell Nucleus
K. Tanabe et al. (31P11-5) ············································································ 102

PR11-6

Establishment of the Chicken Egg Tumor Model for GNCT
K. Matsumoto et al. (31P11-6) ······································································· 103

PR11-7

Evaluation of Antitumor Effectivity on Gd-neutron Capture Therapy with Polymeric
Nanocarries
X. Hou et al. (31P11-7) ··············································································· 104

PR11-8Development of Nano Carriers Installed with Gd(III)-Thiacalixarene Complex for Gd-NCT
T. Yamatoya et al. (31P11-8) ········································································· 105

Project 12 Enhancement of Research Methods for Material Irradiation and Defect Analysis
A. Kinomura (31P12) ··················································································· 107
PR12-1

Study to Improve Transport and Measurement Performance of a Slow Positron Beamline
A. Kinomura et al. (31P12-1)········································································· 108

PR12-2

Electron-irradiation Induced Defects in W-Re
T. Toyama et al. (31P12-2)············································································ 109
Change in the Positron Annihilation Lifetime of Electron-irradiated F82H by Hydrogen
Charging
K. Sato et al. (31P12-3) ··············································································· 110
The Effect of Gamma-ray Irradiation on Luminescence Properties of Collolidal Si Nanocrystals
T. Nakamura et al. (31P12-4) ······································································· 111
Irradiation Technique for Study on Corrosion Resistance of Fusion Divertor Materials
to liquid metal during irradiation
M. Akiyoshi et al. (31P12-5) ········································································ 112
Measurement of Positron Lifetimes of Various Diamond-like Carbon Thin Films
K. Kanda et al. (31P12-6) ············································································· 113
Positron Annihilation Spectroscopy on Diamond-like Carbon Films
S. Nakao et al. (31P12-7) ············································································· 114

PR12-3

PR12-4

PR12-5

PR12-6
PR12-7

Project 13 Chemical and Electronic Properties of Actinide Compounds and their Applications
T. Yamamura (31P13) ·················································································· 116
PR13-1Synthesis and Characterization of Actinide-based Compounds with Honeycomb Layer
Y. Haga et al. (31P13-1) ·············································································· 117v

PR13-2
PR13-3

PR13-4PR13-5
PR13-6

PR13-7

PR13-8Crossover between Fermi-Liquid and Non-Fermi-Liquid States in Th1-xUxBe13 (0 ≤ x ≤ 1)
H. Amitsuka et al. (31P13-2) ···································································· 118
Adsortpion Chracterization of Actinide Chemical Species on Solid Adsorbents- Measurement of Rare Earth Elements by ICP-MS T. Suzuki et al. (31P13-3) ··········································································· 119
Preparation of 228Ra/228Ac Stock Solution
K. Shirasaki et al. (31P13-4) ········································································· 120
Investigation on Complex Formation of Monoamide Compounds with Actinyl Ions
M. Nogami and T. Yamamura (31P13-5)···························································· 121
Consistency Verification between Relativistic Quantum Chemical Calculations andExperiments in Uranium Compounds
M. Abe et al. (31P13-6) ··············································································· 122
Evaluation of Phase Diagram of Minor Actinide Oxides with CALPHAD
H. Shishido et al. (31P13-7) ·········································································· 123
Synthesis of Nobel Phthaloyanine Derivatives and Effect of Substitutent on Recognitionof Light Actinide and Chemical Property
M. Nakase et al. (31P13-8) ··········································································· 124

I-2. COLLABORATION RESEARCHES ··············································································· 125
1. Slow Neutron Physics and Neutron Scattering
CO1-1First Neutron Diffraction Results of Fluoride-ion Battery Materials on VCND
K. Mori and F. Fujisaki (31008) ········································································· 126
CO1-2

Current Status of Versatile Compact Neutron Diffractometer (VCND)
on the B–3 Beam Port of KUR, 2019
K. Mori et al. (31016) ······················································································ 127

CO1-3

Neutron scattering study on microstructure of vitrified radioactive wastes
K. Kaneko et al. (31027) ·················································································· 128
Development of neutron spin flipper with large beam acceptance
M. Kitaguchi et al. (31030) ··············································································· 129

CO1-4
CO1-5
CO1-6

Development of m=6.5 neutron spuermirror on ellipsoidal metal substrate
M. Hino et al. (31109) ····················································································· 130
Development of high spatial resolution cold/ultracold neutron detector
using nuclear emulsion
N. Naganawa et al. (31135) ········································································ 131

2. Nuclear Physics and Nuclear Data
CO2-1
Measurement for thermal neutron capture cross sections and resonance integrals of the243
Am(n,γ)244gAm, 244m+gAm reactions
S. Nakamura et al. (31020) ········································································ 132
CO2-2
Quantitation of Gamma Ray Emission from Caputre Reaction of Uranium-238
Y. Nauchi et al. (31022) ············································································ 133
CO2-3

Development of current-mode neutron detectors for BNCT fields
T. Matsumoto et al. (31102) ........................................................................................... 134

CO2-4

Measurements of thermal neutron total and scattering cross section of moderator materials
J. Nishiyama et al. (31108) ............................................................................................. 135
Measurement of Temperature Depended Themal Neutron Spectrum in Solid Moderator
T. Sano et al. (31156) ..................................................................................................... 136

CO2-5

3. Reactor Physics and Reactor Engineering
CO3-1
Basic Research for Sophistication of High-power Reactor Noise Analysis (II)S. Hohara et al. (31025) ············································································ 137
CO3-2

Demonstration of advanced subcritical measurements: Time-Domain Decompositionbased Integral (TDDI) method and third-order neutron-correlation technique
T. Endo et al. (CA3101) ................................................................................................. 138vi

CO3-3

Measurement of Gamma Ray from Short Lived Fission Product under Background of
Fission Prompt Gamma Ray
Y. Nauchi et al. (CA3102) .............................................................................................. 139

CO3-4

Reactor Noise Power-Spectral Analysis for a Graphite-Moderated and -Reflected Core (II)A. Sakon et al. (CA3104) ............................................................................................... 140
Measurement of fundamental characteristics of nuclear reactor at KUCA (IV)
Y. Kitamura (CA3106) ................................................................................................... 141
Reactor Physis Experiment in Graphite Moderation System for HTGR (II)Y. Fukaya et al. (CA3107) ········································································· 142
Sample Worth Measurements of Lead and Bismuth in Low-enriched Uranium Region at
A-core of KUCA for ADS
M. Fukushima et al. (CA3109) ···································································· 143
Subcriticality Measurement by using a Small Neutron Detector
T. Misawa et al. (CA3110) ............................................................................................. 144
Verification of an Improved Method to Estimate Reactivity
Y. Yamane et al. (CA3111) ............................................................................................. 145
Measurement of Fundamental Characteristics of Nuclear Reactor at KUCA (V)Y. Kitamura et al. (CA3112) ........................................................................................... 146
Measurement of Neutronics Characteristics for Th loaed core at KUCA (II)T. Sano et al. (CA3113) ................................................................................................. 147

CO3-5
CO3-6
CO3-7

CO3-8
CO3-9
CO3-10CO3-114. Material Science and Radiation Effects
CO4-1
Characterization of Additive in Lubricant using Small-Angle X-ray Scattering
Y. Oba (31002) ························································································
CO4-2
Synthesis of alloy nanoparticles in water solution by two steps reduction and one time
γ-ray irradiation
F. Hori et al. (31004) ···············································································
CO4-3
Defects structure and characterization of electron irradiated intermetallic alloys
F. Hori et al. (31005) ···············································································
CO4-4
Magnetic Scattering Contribution in Iron Characterzed by Neutron Diffraction
Y. Oba et al. (31007) ················································································
CO4-5
What Exists in a 2-nm-sized Molecular Caspule Assembeld in Water?
Y.-Y. Zhan et al. (31009) ···········································································
CO4-6
Damage Evolution in Neutron-irradiated Metals during Neutron Irradiation at
Elevated Temperatures
I. Mukouda and Q. Xu. (31041) ···································································
CO4-7
Radiation Resistivity of Ferrite Permanent Magnets Against Neutrons
Y. Iwashita et al. (31042) ···········································································
CO4-8
Elucidation of the Mechanism of the Screw-sense Induction of Polymer Backbone Basedon the Small Angle X-ray Scattering and Dynamic Light Scattering Measurements
Y. Nagata et al. (31051)··············································································
CO4-9
Crystal structure analysis of Abalone shell
K. Iwase and K. Mori (31055) ······································································
CO4-10Radiochemical Research for the Advancement of 99Mo/99mTc Generator by (n, γ) Method (2)Y. Fujita et al. (31065) ···············································································
CO4-11
Radiophotoluminescence phenomenon in Cu-doped silica glasses prepared fromporous silica glass
Y. Takada et al. (31066) ············································································
CO4-12
Study of resonant frequency change with irradiation dose of piezoelectric PZT element
M. Kobayashi et al. (31067) ········································································
CO4-13
Formation of radiation defects on tungsten and their influence on effect ofhydrogen isotope retention
K. Tokunaga et al. (31086) ··········································································
CO4-14
Tritium release behavior from neutron-irradiated FLiNaBe
K. Katayama et al. (31090)··········································································

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CO4-15

Positron Age-Momentum Correlation Mesurements of γ-rays Irradited Polystyrene
H. Tsuchida et al. (31093) ················································································· 162

CO4-16

Formation of nano-structures on Ge surfaces by ion irradiation and study on its formation mechanisms
J. Yanagisawa et al. (31097)········································································· 163
Evaluation of Structural Vacancies in Icosahedral Cluster Solids using Positron Annihilation
J. Takahashi et al. (31100) ··········································································· 164
Absorption Coefficient of Amino Acid in the Sub-THz region using CTR
T. Takahashi et al. (31111)··········································································· 165
Vacancy migration behavior in CoCrFeMnNi high entropy alloys and their subsystems
K. Sugita et al. (31112) ·············································································· 166
Observation of Gamma-ray Induced Current on Coaxial Cable for Analog Data Transfer
Y. Gotoh (31118)······················································································ 167
Correlation between Damage Accumulation by Neutron Irradiation and Hydrogenisotope Retention for Plasma Facing Materials
Y. Oya et al. (31120) ················································································· 168
Complex Structure of Ions Coordinated with Hydrophilic Polymer 20. Ionic
Diffusion in Polymeric Structure Utilized by Polyiodide Ions. (1)A. Kawaguchi and Y. Morimoto. (31122) ························································· 169
A study on destruction of cesium aluminosilicate cage by gamma irradiation (1)H. Ohashi et al. (31128) ············································································· 170
Effects of Buffers and Salts on Nanostructure of Soybean Proteins as Revealed by SAXS
N. Sato et al. (31137)················································································· 171
Porosity Measurements of Sintered-Silver Bonding Plates
K. Wakamoto et al. (31143) ········································································· 172
Differences in the Recovery Behavior of Electron-Irradiation-Induced Vacancies in
Metals with Different Purities
A. Yabuuchi et al. (31157)··········································································· 173
Differences in the Development of Vacancy-Type Defects During Annealing with Different
Irradiated Ion Species
A. Yabuuchi et al. (31158)··········································································· 174
Defect Characterization of Ion-Irradiated GdBa2Cu3O7−δ Superconducting Tapes Probed by a
Slow Positron BeamT. Ozaki et al. (31159) ··············································································· 175
Neutron irradiation tests for ITER plasma diagnostics
M. Ishikawa et al. (31167)··········································································· 176

CO4-17
CO4-18CO4-19CO4-20CO4-21

CO4-22CO4-23CO4-24CO4-25
CO4-26

CO4-27

CO4-28CO4-295. Geochemistry and Environmental Science
CO5-1
Volcanic and Tectonic History of Philippine Sea Plate (South of Japan) Revealedby 40Ar/39Ar Dating Technique
O. Ishizuka et al. (31012) ··········································································
CO5-2
Long Term Observation of Element Concentrations in the Atmospheric Aerosols at
Sakai, Osaka,1995-2017
N. Ito et al. (31024) ·················································································
CO5-3
Ar-Ar dating of submarine basalts
N. Hirano et al. (31039) ············································································
CO5-4
Recrystallization of an amorphous Si layer by H+ ion beam and electron beam irradiation
J. Nakata et al. (31049) ·············································································
CO5-5
Study on Elemental Concentration in the Atmospheric Particulate Matter by INAA
N. Hagura et al. (31052) ···········································································
CO5-6
Neutron activation analysis for sediments, phytoplankton, lake water of Lake Akagi Onuma
Y. Okada et al. (31053) ·············································································
CO5-7
Formation age of Precambrian metamorphic rocks and thermal history
H. Hyodo et al. (31057) ············································································CO5-8
A Study on Evaluation of Redox Condition of Tokyo Bay using Redox Sensitive Elements as
an Indicator by Means of Instrumental Neutron Activation Analysis
M. Matsuo et al. (31061) ···········································································

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184

CO5-9CO5-10
CO5-11

CO5-12
CO5-13

Absorption of alkali metal ions by white radish sprouts
M. Yanaga et al. (31064) ···········································································INAA and Ar-Ar Dating for Micro-sized Extraterrestrail Materials
R. Okazaki and S. Sekimoto (31068) ·····························································
Determination of Abundance of Rare Metal Elements in Seafloor Hydrothermal Ore Deposits by
INAA Techniques-6: Evaluation of analytical accuracy
J. Ishibashi et al. (31077) ··········································································
Research on Earth Surface Processes by Use of Mineral Luminescence
N. Hasebe et al. (31079) ···········································································
Geochemistry of unbrecciated eucrite, Northwest Africa 10962
N. Shirai et al. (31081) ·············································································

185
186

187
188
189

CO5-14

Neutron Activation Analysis of Environmental Samples
Y. Oura and Md. S. Reza. (31088) ································································ 190

CO5-15

Bulk Chemical Compositions of CB and CH Chondrites
M. Ebihara et al. (31091) ··········································································
Determination of Cl, Br and I contents in geochemical reference samples by radiochemical
neutron activation analysis - revisited
M. Ebihara et al. (31092) ··········································································
Spatial Distribution of Halogen Compositions in the Wedge Mantle-derived Metaserpentinite Body inSouthwest Japan
H. Sumino et al. (31113) ···········································································
Fission track age and thermal history of clay deposit of the Tsuchihashi Mine
H. Ohira and Y. Sampei (31119) ···································································
40
Ar-39Ar Dating of Extraterrestrial Materials in KURNS
N. Iwata et al. (31126) ··············································································
Neutron activation analysis of carbonate reference materials: coral (JCp-1) and giant clam
(JCt-1)
S. Sekimoto et al. (31132) ·········································································Long term analysis of Cs isotopic ratio by thermal ionization mass spectrometry
Y. Shibahara et al. (31160) ·········································································
Analysis of Cd and As in the rice seed detected from the remains by NAA
T. Inamura et al. (31165) ···········································································
Ananysis method of strontium in seawater
Y. Ogata et al. (31168) ··············································································INAA using KUR for the determination of elemental content in air particulate samples
J.H. Moon et al. (31169, 31170) ···································································

CO5-16

CO5-17

CO5-18CO5-19CO5-20CO5-21
CO5-22
CO5-23
CO5-24

6. Life Science and Medical Science
CO6-1
Effect of inter-protein interaction on SAXS profile in concentrated MurD solution
H. Nakagawa et al. (31001) ·········································································
CO6-2
Physicochemical study on ILEI suppressing amyloid-β generation
E. Hibino et al. (31003) ··············································································
CO6-3
Structural characterization of circadian clock potein complexes
H. Yagi et al. (31006) ················································································
CO6-4
Interaction between Mint3 and FIH-1 involved in hypoxia stress responses
R. Maeda et al. (31011) ··············································································
CO6-5

CO6-6

CO6-7

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196
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201
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Supramolecular Tholos-Like Architecture Constituted by Archaeal Proteins Without
Functional Annotation
M. Yagi-Utsumi et al. (31013) ······································································ 205
Small Angle X-ray Scattering Measurements on Insulin B-Chain Nucleation
Intermediate Complexed with FibrinogenN. Yamamoto et al. (31028) ········································································· 206
Character of DNA damage induced by nuclear palnt neutron beams
H. Terato et al. (31040) ·············································································· 207ix

CO6-8
CO6-9
CO6-10

CO6-11

CO6-12
CO6-13
CO6-14CO6-15

CO6-16CO6-17
CO6-18CO6-19CO6-20
CO6-21

Radiation-induced clustered DNA damage estimated by homo-FRET analysis
K. Akamatsu et al. (31063) ·········································································· 208
Photoproduction of Medical 18F and 99mTc Isotopes
M. Kurosawa et al. (31069) ········································································· 209
Small Angle X-ray Scattering Measurements on Insulin B chain; a Time-Resolved
Measure-ment to Monitor the Amyloid Fibril Formation via Prefibrillar Intermediates
N. Yamamoto et al. (31070) ········································································· 210
Generation of radioresistant Escherichia coli by adaptive evolution using gamma rays
as selection pressure II
T. Saito et al. (31072) ················································································ 211
Structural study for the nucleosome containing histone variant H2A.B
R. Hirano et al. (31073)·············································································· 212
Effect of High-Intensity Pulsed Coherent Radiation on the Stability of the GeneY. Tanaka et al. (31078)·············································································· 213
Structural analysis of multi-domain protein as studied by complementary use of molecular
dynamics simlulation and small-angle X-ray scattering
R. Inoue et al. (31082) ··············································································· 214
Oligomeric structure and its temperature-dependent change of HspB1 from Chinese hamster
ovary cell
M. Yohda et al. (31083)·············································································· 215
Quantitative analysis of contribution of tumor vascular damage to antitumor effect of
X-ray using BNCR
K. Ono et al. (31095)················································································· 216
Observation of Water Uptake in Alternate Grafting of Tomato and Eggplant Using D2O as Tracer
U. Matsushima et al. (31107) ······································································· 217
Production of medical radioisotopes using electron linear accelerator
S. Sekimoto and T. Ohtsuki. (31131)······························································· 218
N-Acetylneuraminic acid functioned as the scavenger for reacive oxygen species generated
by the gamma-ray irradiation
N. Fujii et al. (31134) ················································································ 219
Preliminary analysis of structural composition of menaquinone-7 produced by Bacillus subtilis natto
T. Chatake et al. (31140)············································································· 220
Measurement of Absorption Spectra of a Humann Calcified Aorta Tissue in the Sub-Terahertz
Region, which Dependented on the Thickness (III)N. Miyoshi and T. Takahashi (31162) ······························································ 221

7. Neutron Capture Therapy
CO7-1
Analyses of the immune-cell reaction and activation mechanisms in the tumor
tissue after boron neutron capture therapy
T. Watanabe et al. (31014) ·········································································
CO7-2
Boron nitride (10BN) a prospective material for boron neutron capture therapy
M. Kaur et al. (31017) ··············································································CO7-3
A Fundamental Investigation on Contents of Important Elements for Activation in
Various Concrete
K. Kimura et al. (31021) ···········································································
CO7-4
Evaluation of the abscopal effect observed by mouse head irradiation following
thermal neutron irradiation
Y. Kinashi and T. Takata (31043) ·································································
CO7-5
The feasiblity study of Eu:LiCAF neutron detector for an accelerator-based BNCT
T. Nakamura et al. (31076) ········································································
CO7-6
Enhancement of the cancer cell-killing effects of boron neutron capture therapy byoverexpression of LAT1 in human cancer cells
K. Ohnishi et al. (31084) ···········································································
CO7-7
Clinical Outcome of BNCT for Advanced or Recurrent Head and Neck Cancer
N. Kamitani et al. (31098) ·········································································
CO7-8
Establichment of a novel mutation breeding using Boron Neutron Capture Reaction (BNCR)
M. Kirihata et al. (31104) ··········································································
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CO7-11
CO7-12
CO7-13
CO7-14
CO7-15

CO7-16

Effects on Dissemination or Invasion of glioma cells by BNCT
N. Kondo et al. (31144) ············································································ 230
iPS cells - derived neuronal cell death and inflammation by thermal neutron irradiation
N. Kondo et al. (31145) ············································································ 231
Resistant Mechanism of Glioma Conferred by Tumor Microenvironment after BNCT
N. Kondo et al. (31146) ············································································ 232
Improvement of the method for analysis of micro boron distribution in tissues
M. Suzuki et al. (31150) ············································································ 233
Development of real-time boron-concentration estimation system for whole-organ-irradiation BNCTY. Sakurai et al. (31151) ············································································ 234
Establishment of protocol for neutron capture therapy for head and neck cancer
I. Ota et al. (31152) ················································································· 235
Anti-tumor evuluation of Gadolinium Neutron Capture Therapy through comparison oftumor size using with polymeric nanocarries
X. Hou et al. (31163) ··············································································· 236
Accelerated deterioration assessment of SOF detector under high neutron flux environment
M. Ishikawa et al. (31166) ········································································· 237

8. Neutron Radiography and Radiation Application
CO8-1
CO8-2

CO8-3
CO8-4
CO8-5

CO8-6

CO8-7
CO8-8
CO8-9
CO8-10
CO8-11
CO8-12

CO8-13
CO8-14CO8-15
CO8-16

Neutron Phase Imaging with Talbot-Lau Interferometer at CN-3
Y. Seki et al. (31019) ···············································································
Study on the Visualization of Organic Matter between Metals to Contribute to the Advancementof the Industrial Products
K. Hirota et al. (31031) ·············································································
Measurements of multiphase flow dynamics using neutron radiography
Y. Saito and D. Ito (31034) ········································································
Visualization of Hydrogen in Pure Palladium via Neutron Radiography and Tomography
K. Shimizu et al. (31036) ··········································································
Visualization and Measurement of Boiling Flow Behaviors in Parallel Mini-channel
Heat Exchanger
H. Asano et al. (31045) ·············································································
Evaluation of Water Distribution and Electrochemical Characteristics in Polymer
Electrolyte Fuel Cell
H. Murakawa et al. (31046) ·······································································
Meltwater Behavior During the Defrosting Process by Using Neutron Radiography
R. Matsumoto et al. (31048) ·······································································
Flow visualization of heavy oil in supercritical water using neutron radiography
T. Tsukada et al. (31074) ···········································································
Analysis of moisture transfer in high-strength concrete embedded rebar exposed to fire
M. Kanematsu et al. (31103) ······································································Development of capillary-plate-based flourescent plates for neutron radiography
T. Sakai et al. (31106) ··············································································
Visualization of a Microchannel Heat Exchanger under Non-uniformly Heated Condition
H. Sakai et al. (31121) ··············································································
Diffusion Measurements on NASICON-Type Structured Lithium Ion Conductors by
Means of Neutron Radiography
S. Takai et al. (31130) ··············································································
Study on the non-destructive nuclide assay for nuclear materials with a self-indication method
J. Hori et al. (31136) ················································································The measurability of photofission reaction of uranium induced by bremsstrahlung photons
K.W. Chin et al. (31155) ···········································································
Distribution of coolant inside a flat laminate vapor chamber in a vertical posture
K. Mizuta et al. (31161) ············································································
Demonstration experiments of an innovative method to detect nuclear material
M. Komeda et al. (CA3108) ·······································································

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9. TRU and Nuclear Chemistry
CO9-1
Leaching behavior of fission products from simulated MCCI debris
T. Sasaki et al. (31015) ············································································· 254
CO9-2
Complex formation of zirconium with hydroxycarboxylic acids
T. Kobayashi et al. (31023) ········································································ 255
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CO9-3

CO9-4
CO9-5
CO9-6
CO9-7

CO9-8

CO9-9

–

Electrodeposition Behaviors of Uranium and Aluminum on Copper Cathode in LiCl-KCl
Eutectic Melts
Y. Sakamura et al. (31035) ·········································································
Structural Change of Borosilicate Glass by Boron Isotope Composition
T. Nagai et al. (31038) ··············································································
Study on leaching behavior of carbon-14 from neutron irradiated stainless steel
R. Nakabayashi et al. (31060) ·····································································
Solvent extraction of selenium in the nitric acid solution with selected elements
T. Kawakami et al. (31062) ········································································
Effect of γ-Ray Irradiation in HNO3 on Adsorptivity of Long-Chain 6-Membered Cyclic
Monoamide Resin
Y. Yoshimura et al. (31114) ········································································
Roll of Electrostatic Interaction in Attachment Process of Fission Products to Solution
Aerosol Particles
K. Takamiya et al. (31139) ·········································································
Precipitation of alkaline earth elements toward the chemical study of Nobelium
S. Hayami et al. (31153) ···········································································

10. Health Physics and Waste Management
CO10-1
Effective Measures on Safety, Security, Hygiene and Disaster Prevention in Laboratories ·T. Iimoto et al. (31018) ·············································································
CO10-2
Scientific Ethnography for Nuclear Science, Part 1-Responsibility of Science, Post 3.11, IItate Village, FukushimaM. Takagaki and S. Masunaga (31033) ··························································
CO10-3
Assessment of non-homogenous exposure of radiation workers in accelerator facility
situation in the small linac facility M. Kowatari and T. Kubota (31050) ······························································
CO10-4
Investigation for valiation of trace elements concentration in accelerator room concrete
G. Yoshida et al. (31056) ···········································································
CO10-5Comparison of Chlorine Concentration in Each Municipal Solid Waste Fraction Measured
by Neutron Activation Analysis and Bomb Calorimeter- Ion Chromatography
K. Ohita et al. (31075) ··············································································
CO10-6
Effect of Ammonium Ion Washing of Radiocesium Contaminated Soil
K. Daiku et al. (31129) ·············································································
CO10-7
Measurement of Radioactivity-Based Particle Size of Radiation-Induced Aerosols
using a Diffusion Battery System in Accelerator Facilities
Y. Oki. (31154) ······················································································
CO10-8
Consideration of radon concentration measurement under natural fluctuation environment
by a new monitor using two filter method
Y. Igarashi et al. (CA3115) ········································································
12. Others
CO12-1
CO12-2
CO12-3
CO12-4CO12-5
CO12-6
CO12-7

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Isotope Dilution-Neutron Activation Analysis for Quantifying Hafnium
T. Takatsuka et al. (31026) ········································································· 271
Study on Superposition of Terahertz Coherent Radiation using a Ring Resonator
N. Sei and T. Takahashi (31029) ·································································· 272
High-count-rate 3He position-sensitive detector readout system
S. Sato et al. (31044) ··············································································· 273
Neutron activation analysis of Ar in titanium metal
T. Miura et al. (31047) ·············································································A response of inner-through type ionizaiotn chamber to 41Ar
A. Yunoki et al. (31059) ············································································Development of neutron imager based on hole-type MPGD with glass capillary plate
F. Tokanai et al. (31080) ···········································································
Gamma ray measurement in the basement of the Kyoto University Research Reactor facility
K. Okada et al. (31089) ············································································

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CO12-8
CO12-9CO12-10CO12-11CO12-12CO12-13CO12-14CO12-15

CO12-16
CO12-17
CO12-18

Neutron efficiency of a two-dimensional neutron detector with MPPC (Mpix)
H. Ohshita et al. (31094) ···········································································
Research on Activation Assessment of a Reactor Structural Materials for Decommissioning (2)M. Seki et al. (31096) ··············································································
Beam Test of a micro-cell MWPC for a muon-electron conversion search experiment, DeeMe
M. Aoki et al. (31105) ··············································································
An attempt to produce carrier free tracer through photonuclear reaction and hot atom effect
T. Kubota et al. (31110) ············································································
Study of Isotope Separation via Chemical Exchange Reaction
R. Hazama et al. (31115) ···········································································
Radius of Gyration of Polymer for Viscosity Index Improver at Various Temperatures
Evaluated by Small-Angle X-Ray Scattering
T. Hirayama et al. (31116) ·········································································
Friction Reduction by the Combination Use of MoDTC and Organic Friction Modifier
T. Hirayama et al. (31117) ·········································································
Multi-element neutron activation analysis of selected Japanese food samples byneutron activation analysis
M. Fukushima et al. (31123) ·······································································
Installation of Flowing Sample Neutron Activation Analysis at KUR
M.A. Soliman et al. (31138) ·······································································
Neutron Resonance Spectrometry of Urinium for Nuclear Security and Safeguards Education
J. Kawarabayashi et al. (31141) ···································································
Evaluation test of SEL recovering system used in CubeSat by using 252Cf
H. Masui et al. (31142) ·············································································

II. PUBLICATION LIST (April 2019 – March 2020)

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3URMHFW5HVHDUFKRQ1XFOHDU6SHFWURVFRS\DQG&RQGHQVHG0DWWHU
3K\VLFV8VLQJ6KRUW/LYHG1XFOHL
polarization of γ-rays from short-lived β decaying nuclei
using a clover detector (the same detector that M. Shibata
HW DO. used in 31P1-2) as a Compton polarimeter andadditional coaxial Ge detectors in order to obtain themultipolarities of those γ-rays. In the last period, they
confirmed the feasibility of their polarimeter systemusing the established 258-410 keV E2-E2 γ cascade in146
Ce arising from 146La via E decay, available at
KUR-ISOL. In this period, they succeeded in obtaining
the preliminary result showing the E2 character of the1358-keV γ ray from 148Pr (half-life of 2.1 m) decaying to148
Nd, produced at KUR-ISOL. 
Ultrafine bubbles, attracting a lot of attention invarious industrial fields, are of the diameter less than one
micro meter. Despite the Young-Laplace equation
predicting a high internal pressure for such a small
bubble in water so that it should survive only very shorttime, it is reported to survive more than a month.
Employing the time-integral perturbed angularcorrelation (TIPAC) technique for 125I arising from 125Xe(half-life of 17 h) produced at the slant exposure tube of
KUR, M. Tanigaki HW DO. successfully obtained theinternal pressure of ultrafine bubbles of the average
diameter about 200 nm containing Xe gas inside, thevalue of which is much smaller than that theYoung-Laplace equation predicts. In this period, they
(31P1-5) reevaluated the value of the time-integrated
perturbed angular correlation.
A perovskite manganese oxide La0.7Ca0.3MnO3 (forshort, LCMO) is well known to exhibit colossal
magnetoresistance. It is considered that polaron dynamics
plays a significant role in this phenomenon. Because of
the large variation in physical properties of La1-[Ca[MnO3
with [, the $-site (La or Ca) information is especially
important. In order to obtain this local information for
LCMO, W. Sato HW DO (31P1-6) synthesized 2 at. %nonradioactive Cd-doped LCMO containig a tracer
amount of radioactive 111mCd (half-life of 49 m) producedin the pneumatic tubes of KUR and took 111Cd(←111mCd)
TDPAC (time-differential perturbed angular correlation)
spectra at temperatures above and below the Curie
temperature of ~ 250 K. They succeeded in observing thestatic and dynamic polarons around the probe nuclei atthe $ site of LCMO.
SrTiO3 is a cubic perovskite oxide. Doped with metal
impurity ions, it exhibits a wide variety of electronic
properties. In order to obtain local information on the
impurity site, S. Komatsuda HW DO. (31P1-7) synthesized
SrTiO3 containing a tracer amount of commerciallyavailable 111In (half-life of 2.8 d) and took theroom-temperature TDPAC spectrum of 111Cd arising from111
In. They found three kinds of quadrupole frequencies
in the spectrum: one is zero frequency indicating 111Cd atthe defect-free substitutional site and the other two
non-zero frequencies implying 111Cd at the substitutionalsite associated with oxygen vacancy.

Y. Ohkubo,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\ 
2EMHFWLYHDQG3DUWLFLSDWLQJ5HVHDUFK6XEMHFWVThe main objectives of this project research are theinvestigation of the nuclear structure of unstableneutron-rich nuclei and also the local properties ofmaterials using short-lived nuclei.
This period is the third and last year of the project.
The research subjects reported here are as follows:
31P1-1 Technique of transferring radioactive atomic
nuclei implanted in dry ice film
31P1-2 β––Decay spectroscopic studies of fission
products using the clover detector
31P1-3 Linear polarization measurement for γ rays from148Pr
31P1-5 Measurement of the internal pressure in ultrafine
bubbles by angular correlation technique
31P1-6 Temperature-dependent polaronic local structuresin La0.7Ca0.3MnO3 observed through spin relaxation of
TDPAC probe nuclei
31P1-7 Local structure of In impurities doped in SrTiO3
studied by TDPAC method
0DLQ3RLQWV'HVFULEHGLQWKH5HSRUWVLQWKH)ROORZLQJ
6L[SDJHVAs a means to measure the charge distribution of an
unstable nucleus, it is promising to make a muonic atomcomposed of the nucleus that are trapped in deuterium
film and then to measure the energies of X-ray emitted
from the muonic atom. However, it is unavoidable to deal
with high radioactivity. One of the technical problems is
how efficiently and safely long-lived radioactivity in theapparatus is removed after such an experiment is done. A.
Taniguchi HWDO. (31P1-1) has attacked this problem using
a beam of 146LaO+ radioactive ions available at
KUR-ISOL and an apparatus designed for the present
work. In this period, they improved the apparatus so thatthe removal efficiency became much higher than thatobtained previously.
M. Shibata HW DO. (31P1-2) investigated the levelstructures of 153Nd and 154Nd, arising via E decay,
respectively, from 153Pr (half-life of 4.3 s) and 154Pr(half-life of 2.3 s), fission products of 235U + thermal
neutron, available at KUR-ISOL. Because of the large 4E
values, 5752 keV for 153Pr and 7790 keV for 154Pr, it ispossible to access to high excited levels of 153Nd and154
Nd. They used a clover detector consisting of 4 Ge
crystals both in singles and add-back modes. For 153Nd,
they identified eight new excited levels and also newnineteen J-rays. The detailed analysis is in progress forconstructing the decay schemes.
Y. Kojima HW DO. had tried to measure the linear

31P1

‑3‑

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35
A. Taniguchi, P. Strasser1, M. Tanigaki and Y. Ohkubo

the absolute trap efficiency for the implanted radioactivities is in progress, the higher transfer efficiency result of
about 880% was obtained (see Fig.1). The efficiency isdefined as the ratio of the radioactivities on the trap tothose remaining on the catcher, which was deduced fromthe peak counts of 454 keV J-ray of 146Pr by taken into
account of the detection efficiency of each Ge detector in
its actual arrangement. This result is still poorly reproducible and the appropriate parameters for film formation have not yet been fixed, but much higher than theprevious results [4]. Therefore, it can be said that thecontrol of the vacuum degree is one of the importantparameters.
$&.12:/('*0(176 This research was partially
supported by the Ministry of Education, Science, Sports
and Culture, Grant-in-Aid for Scientific Research (C)(24540303, Akihiro Taniguchi, and 15K05103, Akihiro
Taniguchi).
5()(5(1&(6[1] I. Angeli and K.P. Marinova, At. Data Nucl. Data
Tables (2013) 69-95.
[2] P. Strasser HW DO., Hyperfine Interact.  (2009)121-127.
[3] A. Taniguchi HWDO., KURRI Prog. Rep. 2013, p98.
[4] A. Taniguchi HWDO., KURNS Prog. Rep. 2018, p28.

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10

4

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3

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1

Counts,1752'8&7,21 Measurement of the emitted X-ray
energy from muonic atoms is a powerful method for theinvestigation of the nuclear charge radius [1]. Recently, a
new method using solid hydrogen film has been developed to produce muonic atoms. In this method, negative
muons are injected to solid deuterium film in which nuclei of interest are implanted beforehand, thereby muonicatoms being formed through the highly-efficient muontransfer reaction. The feasibility of this method wasdemonstrated and promising results were obtained [2]. In
this study, one of the problems in applying this method tounstable nuclei, concerned with handling of residual radioactivities in deuterium film after experiments, in particular their highly efficient recovery, was approachedusing a radioactive-isotope beam from KUR-ISOL anddry ice film instead of solid hydrogen film.
(;3(5,0(176 An apparatus capable of implanting
radioactivities to dry ice film was installed at the beamline of KUR-ISOL [3]. This apparatus has two coolable
copper blocks and one CO2 gas diffuser in the vacuum
chamber. Dry ice film is formed on the surface of one
cooled block (catcher) by sprayed CO2 gas through the
diffuser and radioactivities are implanted into it. In aseries of recent experiments, even if films of the same
appearance were formed on the catcher, large variations
were observed in the amounts of radioactivities transferred to the other block (trap). It is considered that thecondition of dry ice film is important and the forming
parameters should be controlled more finely in order toimprove the reproducibility of the transfer efficiency. In
this work, film was formed while recording the vacuum
degree in the chamber with a data logger. In addition, byattaching "standing collars" on the four sides of the film
formation surface, more CO2 gas from the diffuser isguided to the surface during film formation, furthermore
during transfer, the collars cover the catcher-trap gap sothat sublimation components become less likely to escape into the chamber. About 106 ions of 146LaO+ were
implanted into dry ice film on the catcher in every run.
After the implantation, the other pre-cooled trap was
moved to the frontal vicinity of the catcher, and then thecatcher was warmed by stopping LN2 flow. With thisprocedure, the atoms of 146Ce and 146Pr were released
from the catcher and were re-trapped on the trap together
with CO2. The transfer efficiency was measured by detecting the J-rays emitted from each of the blocks. In
each run, it took about 2 hours from the implantation to
the completion of the transfer.
5(68/76 $1' ',6&866,21 The transfer efficiencies were measured by changing the amount of CO2
while confirming the vacuum degree when dry ice films
were formed. Although the detail data analysis including

(a)

10

1

0

Pr 735.7

Pr 788.6

146

Pr 601.1

Annihilation J

400
Gamma ray energy (keV)

146

2

146

Counts

10

146

(c)

Pr 453.9

3

146

10

Ce 316.7

1

146

10

Ce 218.2

2

146

10

Ce 264.6

Counts(b)

800

Fig.1 Transfer of radioactivities using a cold trap type
recovery apparatus. (a)Gamma-ray spectrum of the catcher immediately after 146La implantation. 146La (71/2 = 10 s
and 6 s) decayed out and J-rays of 146Ce (71/2 = 14 m) and146
Pr (71/2 = 24 m) were observed. Gamma-ray spectra of(b) the catcher and (c) the trap after the transfer.

31P1-1‑4‑

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235
U. A 72 mg of 93% enriched UF4 was irradiated with athermal neutron flux of 31012 Q/cm2/s. The radioactive
sources were collected on a thin Mylar tape and were

31P1-2
‑5‑

246.5

227

169

134.5



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

79.5

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0
1500

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994

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895.6

,1752'8&7,21 Precise decay scheme of fission
products are very important to study nuclear structure andalso decay heat evaluation in nuclear reactor. The neutronrich and short-lived nuclei around mass number 150 have
low yields then their decay data are scarcely studied. In
particular, 153Pr (T1/2 = 4.3 s) and 154Pr (T1/2 = 2.3 s) werestudied by separating from the fission products of 235U
with isotope separator on-lines (ISOL) and was reported
few Ȗ-rays[1, 2], nevertheless, the 4ȕ-value of them arereported to be 5762 and 7790 keV [3], respectively. Itmeans that the both daughter nuclei are expected to havemuch higher excited levels and also isomeric states having
Ps order of half-lives. To identify higher levels and highenergy Ȗ-rays and to propose detailed decay scheme, the Jrays associated with the E-decay of 153Pr and 154Pr were
measured with a clover detector at KUR-ISOL.
The clover detector has 4 large Ge crystals of 80 mm indiameter and 90 mm in length, they are arranged as theshape of a four-leaf clover, and it has through-hole whichdiameter is 15 mm in the detector. The solid angle is 98%
in center of the hole, so Ȗ rays can be measured with highefficiency. The list mode including time information, socalled a time-stamped list mode, data acquisition (DAQ)
system was adapted to identify the J-J coincidence relation.
With this system, two types J-ray spectra, those are“singles” and “add-back“ spectra can be obtained by offline analyses. In the add-back spectra compared withsingles spectra, sum peaks are strongly observed, on theother hand, the cascading Ȗ rays are observed weakly bycoincidence summing out. The off-line analyses, thelocation of J rays in the decay scheme can be made clear.
To deduce the half-lives of isomers with the DAQ system,
E-J time difference method was applied. In this method,
the time difference between the J-ray of interest and acertain continuum part of spectrum which corresponds Erays are extracted from the list mode data. In this method,
the counting rate during the measurement is an importantparameter for obtain reliable results. The isomer (T1/2 =52.6 μs) at 1088 keV in 95Y of daughter 95Sr (T1/2 = 23.9 s)
is proper nucleus to check the effect of the counting rate on
the obtained value.
(;3(5,0(176 The nuclei of interests were massseparated by the KUR-ISOL from the fission products of ND

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periodically transported to the center of the detector withcomputer-controlled tape moving system. The tape moved
periodically with two times of each half-life. In thethrough-hole of the detector, the two semicircle-formed
6mm thick acrylic sticks were set on the both side of Mylar
tape as ȕ-ray absorbers. The detector was shielded with 10
cm thick lead bricks and 5 cm thick boron-doped
polyethene bricks. The data were recorded in the DAQ
system of APV8008 and APV8016 made by Techno AP
Corporation. The measurements of 153Pr, 154Pr and 95Sr
were performed for 8, 11 and 8 hours, respectively.
5(68/76 Here, the preliminarily result of eachexperiment was briefly described. Concerning 154Pr, atypical coincidence spectrum gated by the 162.4 keV Ȗ-ray,which were previously reported in ref [1], is shown in
Fig.1. Ten J-rays including previously proposed the 70.8,
794.4 and 895.6 keVJ-rays [1] and Nd Kx-rays were incoincidence with the 162.4 keV Ȗ-ray. In addition, the sum
peak of 162.4 + 169 keV was observed in the add-back
spectrum, it means they are cascade relation each other.
Concerning 153Pr, eight excited levels and nineteen Ȗ-rays
were newly identified in addition to the previous result [2].
The half-life value of isomeric state of 191.7 keV wasdetermined to be 1.13(10) Ps with the E-J time difference
method. This value is in agreement with the previous valueof 1.06(5) Ps.
From the results of the half-life of the 1088 keV level in95m
Y through theE-decay of 95Sr by the E-J time differenceis method, the higher counting rate is, the shorter the result
became. It was found desirable to keep the count rate
below 5 kcps in this method.
Further analyses for construction of the decay schemes of
153
Pr and 154Pr are in progress.

794.4
799.5

Y.Ishikawa, M. Kanaji, Y. Irie1, T. Yamaguchi1,
M. Shibata2,H. Hayashi3 and A. Taniguchi4

Counts/Channel

35

400
1900

500
2000

Fig. 1. Coincidence spectrum gated by the 162.4 keV Ȗ-ray inthe decay of 154Pr. The closed circles indicate the reported Ȗrays [1].

5()(5(1&(6>@ Y. Toh HWDO, Z. Phy. A 355, (1996)
>@ S. Yamada HWDO., J. Phys. Soc. Jpn. 65, (1996)
>@ The 2016 Atomic Mass Evaluation.
http://amdc.impcas.ac.cn/web/masseval.html

35

/LQHDU3RODUL]DWLRQ0HDVXUHPHQWIRUJ5D\VIURP3U

Y. Kojima, H. Sawai1, Y. Ishikawa1, M. Kanaji1, Y. Irie2,
T. Yamaguchi2, A. Taniguchi3 and M. Shibata

5(68/76 The list data were analyzed using an off-line
sorting program. In this analysis, we considered data recorded within 460 ns as a coincident event, and focused on
the 302-451 keV and 302-1358 keV J-ray cascades. The
former cascade is known as an E2-E2 transition, while
the multipolarity of the 1358 keV J ray in the latter cascade is unknown. The 1358-keVJ ray is a transition froma 2+ to a 2+ level, so that the multipolarity is expected tobe M1 or E2.
From coincidence spectra gating on the 302-keV J ray,we obtained the asymmetry value $ of 0.045(17) for the
451-keV J ray. Because the theoretical value of polarization 3 is 0.1667 for the E2-E2 cascade in the 4+-2+-0+
spin-parity sequence, the sensitivity 4 was found to be 4
= $/3 = 0.27(10). As shown in Fig.1, this 4-value agrees
with those obtained in the previous experiments. For the1358-keV J ray, the asymmetry value of $ = 0.008(15)was observed. Because the sensitivity is about 0.16 for
1358 keV (Fig.1), the degree of polarization was deduced
to be 0.05(10). Here, the theoretical 3-values are 0.43
and 0.08 if the 1358-keV J ray is a M1 and E2 transition,
respectively. Our result favors the multipolarity of the1358-keV J ray is E2, while the experimental uncertainty
is large.
&21&/86,216 Compton scattering asymmetries
were observed for J rays from 148Pr. The result suggests
the 1358-keV J-ray is an E2 transition.

5DGLRLVRWRSH5HVHDUFK&HQWHU1DJR\D8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ1DJR\D8QLYHUVLW\
6FKRRORI(QJLQHHULQJ1DJR\D8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 Gamma-ray multipolarities are oneof the most important properties for nuclei because they
are necessary in discussion of nuclear structures. For determination of the J-ray multipolarities, the linear polarization is useful, and is usually measured using an asymmetry of Compton scattering events. In recent years, weare trying the linear polarization measurements for
short-lived E-decaying nuclei using a clover HPGe detector [1]. The clover detector consists of four large Ge
crystals packed closely, and the size of each crystal is 80
mm in diameter and 90mm in length. In this technique, aCompton scattering asymmetry $ in orthogonal directions is determined by means of coincidence measurements. After correcting the $-value using the polarimeter
sensitivity 4, the value of $/4 is compared with the degree of polarization which has been calculated for various
multipolarities.
In AY2018, we tried linear polarization measurements
for 146La produced by on-line isotope separator
KUR-ISOL [2], and succeeded in observation of theCompton scattering asymmetry for 258-410 keV E2-E2 J
cascade. In this report, we present the preliminary results
obtained for 148Pr.
(;3(5,0(176 The detection system consisted of theclover detector as a polarimeter, a coaxial 60% (relative
efficiency) HPGe detector as a directional detector, and acoaxial 38% HPGe detector to deduce correction factorsof detection efficiencies. The directional detector wasplaced perpendicular to the clover detector, and was used
to define a UHIHUHQFHSODQH. A detector-to-source distancewas 10 cm for all detectors. The preamplifier signals
from the detectors were processed by a VME-based dataacquisition system, and the data on the pulse height andthe detection time were recorded in event-by-event mode.
Gamma rays from the E  decay of 148Pr (half-life of
2.1 min) were measured at KUR-ISOL. The 148Pr nuclei
were produced by the thermal-neutron-induced fission of235
U. The fission products thermalized in the target
chamber were transported by a He-N2 mixture gas jet
stream to a surface-ionization-type ion source. After ionization to the chemical form of 148Pr16O+, the nuclei wereextracted, accelerated to 30 keV, and mass-separated. The
mass-separated beams were implanted into an aluminized
Mylar tape in a tape transport system. The source wasperiodically moved to a detector port with time intervalsof 220 s. The measuring times were 73 h and 11 h under a
1-MW and 5-MW operation condition, respectively.

Sensitivity 4

0.5

0.3

0.1

500

1000
Energy (keV)

Fig. 1. Energy dependence of the polarization sensitivity. Open and filled marks show data obtained inthis experiment and previous measurements using
60
Co, 134Cs, 152Eu and 146La [3], respectively. The
curve is only a guide to the eye.
5()(5(1&(6>@ Y. Shima HWDO., Appl. Radiat. Isot. (2014) 97-103.
>@ A. Taniguchi HWDO, Nucl. Instr. and Meth. A, (1994)378-382.
>@ Y. Kojima HWDO., KURNS Prog. Rep. 2018. PR3-3.

31P1-3‑6‑

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W. Sato1, 2, S. Komatsuda3, H. Shimizu2, R. Moriichi2, S.
Abe1,2, S. Watanabe2, S. Komatsu2, T. Terai4, S. Kawata5,
and Y. Ohkubo6

angular correlation as a function of the time interval of
the cascade Ȗ-ray emissions by the following expression:

A22G22 (t) =,QVWLWXWH RI 6FLHQFH DQG (QJLQHHULQJ .DQD]DZD
8QLYHUVLW\*UDGXDWH6FKRRORI6FLHQFHDQG7HFKQRORJ\.DQD]DZD
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8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ2VDND8QLYHUVLW\
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2[N(π ,t) − N(π /2,t)] ,N(π ,t) + 2N(π /2,t)(1)

where $22 denotes the angular correlation coefficient,*22(W) the time-differential perturbation factor as afunction of the time interval W between the cascade Ȗ-rayemissions, and 1(θ, W) the number of the delayedThe
coincidence events observed at an angle θ.
measurements were performed at different temperatures.
5(68/76: The TDPAC spectra of 111mCd(→111Cd)
embedded in LCMO are shown in Fig. 1. We found thatthe room-temperature spectrum consists of two different
components reflecting a distorted and a less distorted
sites having the fractional ratio of 7 : 3. The ratio agrees
with that of Mn3+ and Mn4+ abundances, suggesting thatthe former local distortion arises from JT polarons
formed by localized HJ electrons on Mn3+ ions. This
inference is supported by the observation that theoscillatory structure of the distorted component
completely disappeared from the spectra at 201 K and 77
K (< 7&). The disappearance of the oscillation of the
distorted component below 7& can be explained by thefast relaxation of the probe nucleus caused by fluctuationof the polaronic local lattice dragged by the conduction
electrons in the ferromagnetic metal phase. At heliumtemperature, however, the TDPAC spectrum consists of asingle component with an averaged quadrupole frequency,
indicating freezing of the fluctuation. This observationsuggests that the lattice can no longer follow the electron
movement at this low temperature. The present workshows significance of nonmagnetic probes in the study of
local fields in magnetic materials.

,1752'8&7,21: It is well known that a perovskite
manganese oxide La0.7Ca0.3MnO3 (LCMO) exhibits theeffect of colossal magnetoresistance, and it has received
high expectations for application to a variety offunctional magnetic materials.
For its practicalapplication, it is essential to investigate themagnetotranport phenomenon of the oxide by obtaining
information on the local field at each site on an atomic
scale in addition to its bulk properties. Especially, the $site
informationisvery
importantbecausemagnetoresistance of R1-[A[MnO3 is governed largely by
doping of $-site ions. For a detailed investigation of the$-site field, we employed time-differential perturbed
angular correlation (TDPAC) spectroscopy with the111m
Cd(→111Cd) probe [1]. Because the ionic radius of
the Cd ion is close to those of La and Ca, the probe
nucleus can selectively occupy the $ site, which allows
us to observe the change of the local fields attemperatures above and below 7& (~ 250 K). In thepresent work, we report a successful observation of
dynamic motion and freezing of Jahn-Teller (JT) polarons
formed by HJ electrons on Mn ions.




EXPERIMENTS: Stoichiometric amounts of La2O3,
MnO2, and CaCO3 were mixed well in a mortar, and thepowdery mixture was calcined at 1273 K for 12 h. The
sample was again ground to uniformity, and it waspressed into a disk. The disk was then sintered at 1473
K for 96 h. Successful synthesis of LCMO wasconfirmed by powder X-ray diffraction patterns andmagnetization measurements.
Neutron irradiation was performed for cadmiumoxide (CdO) enriched with 110Cd in Kyoto University
Reactor to produce radioactive 111mCd by a neutron
capture reaction. The radioactive Cd(111mCd)O powder
was mixed well with the LCMO prepared in advance, andthe pressed disk was sintered in vacuum at 1373 K for 45
min. TDPAC measurements were carried out for the111m
Cd(→111Cd) probe on the 151-245 keV cascade Ȗ rays
with the intermediate state of ,= 5/2 having a half-life of
85.0 ns. In the present work, we obtained the perturbed

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Fig. 1. TDPAC spectra of 111mCd(→111Cd)
La0.7Ca0.3MnO3 measured at temperatures indicated.

in

REFERENCE:[1] W. SatoHWDO Phys. Rev. B,  (2019) 184111(1-7).

31P1-6

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S. Komatsuda, W. Sato1 and Y. Ohkubo2*22 (W)=V2,0 + ෍ V2,Q cos(ZQ W) .

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YHUVLW\1,QVWLWXWHRI6FLHQFHDQG(QJLQHHULQJ.DQD]DZD8QLYHUVLW\2,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\

(2)

Q=1

For all symbols in eq.(2), refer to our previous paper[2].
The spectrum in Fig. 1 can be reproduced by a fit withthree unique quadrupole frequencies. As for one of thesecomponents, the quadrupole frequency shows a zero. On
the basis of the cubic structure of SrTiO3, this signifies the111
Cd(←111In) probes occupy defect-free substitutional Sr
or Ti sites in SrTiO3. The remaining two components
shows two well-defined EFG values which is characterized by the quadrupole frequencies and its distributions
Z41 = 48.9(1) Mrad/s, G1 = 0%and Z42 = 52.1(2) Mrad/s,
G2 = 0%, respectively. These non-zero frequencies imply
that defects were associated with 111In probes. It has already been reported that the oxygen vacancy is formed bysubstitution of trivalent metal ions such as Fe3+ ion into
Ti4+ for charge compensation [3]. Therefore, we assume
that part of the 111In probes is associated with the oxygen
vacancy, substituting at Ti or Sr site. For more information on the microstructure of SrTiO3, TDPAC measurements with 111Cd(Ћ111mCd) probe are now in progress.

,1752'8&7,21  Strontium titanate (SrTiO3) is a cubic perovskite oxide. SrTiO3 doped with metal ions as
impurities exhibits a wide variety of electronic properties.
Especially, SrTiO3 doped with trivalent metal ions at Ti4+
site has been attracted much attention because of their excellent photocatalytic activity [1]. For a practical use of
SrTiO3, it is necessary to obtain more microscopic information on the impurity site. Therefore, we investigatedthe local structures at the In3+ site in SrTiO3 by means of
the time-differential perturbed angular correlation(TDPAC) method using the 111Cd(Ћ111In) probe.
(;3(5,0(176 Polycrystalline SrTiO3 sample wasprepared from stoichiometric mixture of SrCO3 and TiO2.
The powders were mixed in a mortar and pressed into a
disk. For TDPAC measurements, commercially available 111In solution was added in droplets onto the disk.
The disk was sintered in air at 1473 K for 24 h for preparation of doped SrTiO3 sample. It was confirmed fromthe powder XRD pattern for the nonradioactive sample
that calcination at 1473 K for 24 h is sufficient to synthesize a single phase SrTiO3. The TDPAC measurement
was carried out for the 171-245 keV cascade J rays of111
Cd(Ћ111In) probe with the intermediate state of , = 5/2
having a half-life of 85.0 ns.

$22*22 (W)

5(68/76 Figure 1 shows the TDPAC spectrum ofCd(Ћ 111In) probe in SrTiO3. The measurement was
performed at room temperature. The directional anisotropy on the ordinate, $22 *22 (W), was deduced with thefollowing simple operation for delayed coincidence eventsof the cascade:





111

$22*22 (W )2 [ 1 (S , W )㸫1 (S / 2, W )].
1 (S , W )  2 1 (S / 2, W )












Time (ns)Fig. 1. TDPAC spectrum of 111Cd(Ћ111In) probe in
SrTiO3 at room temperature. The line is the result ofa least-squares fit with eq.(2).

(1)

Here, $22 denotes the angular correlation coefficient,*22 (W) the time-differential perturbation factor as a function of the time interval, W, between the relevant cascade Jray emissions, and 1(T,W) the number of the coincidence
events observed at angle, T. The oscillatory structure observed in Fig.1 reflects electrostatic interactions between
the probe nucleus and the extranuclear field because thesample consists of no magnetic materials. We thus performed a least-squares fit to the spectrum in Fig. 1 with
*22(W) expressed as

5()(5(1&(6>@ Y. Goto HWDO., -RXOH (2018) 509-520.
>@ S. Komatsuda HWDO., -$SSO3K\V (2014) 183502
1-5.
>@ J. S. Yoon. HWDO., (OHFWURQ0DWHU/HWW (2011)209-213.

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Project Research of Accelerator-Driven System with Spallation Neutrons at
Kyoto University Critical Assembly

C. H. Pyeon, M. Yamanaka, K. Hashimoto, N. Aizawa,A. Oizumi, M. Fukushima, G. Chiba, K. Watanabe and
T. EndoInstitute for Integrated Radiation and Nuclear Science,
Kyoto University

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Atomic Energy Research Institute, Kindai University
Graduate School of Engineering, Tohoku University

Nuclear Science and Engineering Center, Japan Atomic
Energy AgencyGraduate School of Engineering, Hokkaido University
Graduate School of Engineering, Nagoya University

INTRODUCTION: At the Kyoto University Critical
Assembly (KUCA), a series of the accelerator-driven
system (ADS) experiments [1]-[6] had been carried out
with the combined use of A core (solid-moderated and-reflected core) and the fixed-field alternating gradient(FFAG) accelerator. Project research of “Accelerator-Driven System with Spallation Neutrons at Kyoto
University Critical Assembly” was composed of six research teams in domestic: Kindai University; Tohoku
University; Japan Atomic Energy Agency (JAEA); Hokkaido University, Nagoya University; Institute for Integrated Radiation and Nuclear Science, Kyoto University(KURNS). In the project research organized by KURNS,
the ADS core was comprised of two zones: test zone (f)of low-enriched uranium (LEU composed of highly-enriched uranium and natural uranium) modeling coreand driver zone of normal core (F: 1/8”p60EUEU) core,
as shown in Fig. 1. Also, 100 MeV protons generated by
the FFAG accelerator were injected onto the lead-bismuth(Pb-Bi) target. The objectives of the project researchwere to examine experimentally neutron characteristicsof the LEU modeling core in ADS, and to investigate
applicability of current measurement technologies to kinetic parameters and numerical methodologies to deterministic and stochastic calculations, in the ADS experiments with spallation neutrons at KUCA.
EXPERIMENTS: In the ADS experiments with spallation neutrons, main characteristic of proton beams by the
FFAG accelerator were shown as follows: 100 MeV energy; 30 Hz frequency; 100 ns repetition rate; 30 pA to 1
nA intensity; 40 mm diameter beam spot. The research
topics were revealed in each research team as follows:- Subcriticality measurement by the noise method(Kindai University)- Measurement of reaction rate of intermediate neutrons(Tohoku University)- Am-243 irradiation (JAEA and Hokkaido University)- On-line monitoring of kinetic parameters(Nagoya University)- Neutronics of LEU modeling core in ADS(Kyoto University)

31P2

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Fig. 1. Top view of core configuration with LEU test andEE1 driver zones at KUCARESULTS: From the results of a series of ADS experiments, special attention was made to the following items:
applicability of the noise method to subcriticality measurement in ADS with spallation neutrons (Kindai); effectof intermediate neutrons for reaction rates in ADS(Tohoku); feasibility study on Am-243 irradiation at a
critical state (JAEA and Hokkaido); applicability of advanced measurement system with optical fibers to on-line
monitoring of kinetic parameters (Nagoya); benchmarks
on kinetic parameters in LEU modeling core of ADS withspallation neutrons (Kyoto).
CONCLUSION: The project research of ADS withspallation neutrons at KUCA was successfully conductedwith the combined use of LEU modeling core and FFAG
accelerator at KUCA. A series of static and kinetic ADS
experiments revealed importantly applicability of current
measurement methodologies to upcoming actual ADS
facilities in the future, demonstrating remarkable reconstruction of ADS experiments by numerical calculations.
REFERENCES:[1] C. H. Pyeon, et al., J. Nucl. Sci. Technol., 46, (2009)1091-1093.
[2] C. H. Pyeon, et al., Nucl. Eng. Technol., 45, (2013)81-88.
[3] C. H. Pyeon, et al., Nucl. Technol., 192, (2013)
181-190.
[4] C. H. Pyeon, et al., Ann. Nucl. Energy, 105, (2017)346-354.
[5] C. H. Pyeon, et al., J. Nucl. Sci. Technol., 55, (2018)
190-198.
[6] C. H. Pyeon, et al., J. Nucl. Sci. Technol., 57 (2020)
133-135.
[6] M. Yamanaka, et al., J. Nucl. Sci. Technol., 57 (2020)
205-215.

35 6XEFULWLFDOLW\0RQLWRULQJIRUD5HDFWRU6\VWHP'ULYHQE\6SDOODWLRQ6RXUFH ,,, 
K. Hashimoto, A. Sakon, S. Hohara, K. Nakajima1, K.
Takahashi1,C. H. Pyeon2, T. Sano, M. Yamanaka2$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\*UDGXDWH6FKRRORI6FLHQFHDQG(QJLQHHULQJ.LQGDL8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Feynman-α and Rossi-α Methods
have been frequently employed to determine subcritical
reactivity of nuclear reactor systems driven by Poisson
source such as Am-Be neutron source. Recently many
advanced formulas for a pulsed non-Poisson source suchas spallation source have been derived. The objectives ofthis study are to confirm experimentally an applicabilityof these formulas for a subcritical reactor system driven
by a spallation source and to investigate some
non-Poisson character of spallation neutron source.

Fig.1. Y obtained by Feynman-α analysis.

(;3(5,0(176A subcritical system was constructed on the A loading of the Kyoto University Critical
Assembly. The system had a lead-bismuth target, towhich 100Mev proton beam was drawn to cause spallation reactions. The repetition frequency of the proton
pulse beam was 30Hz. Time-sequence counts data fromfour BF3 proportional counters were acquired for 30
minutes at several subcritical states referred to as A~F.
The subcritical reactivity was adjusted by axial positionsof 3 control rods, 3 safety rods and a central fuel loading.
Fig.2. Prompt-neutron decay constant.
5(68/76 Figure 1 shows a Feynman-α analysis result obtained from a counter B1 placed near the reactor
core. The Degweker’s formula [1] , where a non-Poisson
character and a delayed neutron contribution were considered, were fitted to these Y data to determine theprompt-neutron decay constant α. These fitted curves arein very good agreement with the Y(T). As shown in Figure 2, the decay constants α determined by the present
Feynman-α analysis is consistent with that obtained under stationary inherent neutron source, except for counter
B4. Only the decay constant obtained by counter B4 has alarge difference. This is because the counter B4 is placed
far from the core and closely to a spallation target.
Figure 3 shows a subcriticality dependence of prompt
correlation amplitudes obtained by respective Feynman-αanalyses under stationary inherent source and spallation
source. Clearly, the present non-Poisson spallation enhances the correlation amplitude, compared with the
Poisson inherent source. A non-Poisson Character is responsible for this enhancement.

Fig.3. Feynman-α correlation amplitude enhanced bynon-Poisson spallation source.
5()(5(1&(6[1]Y.S. Rana, S.B. Degweker, Nucl. Sci. Eng., (2009)
117-133.

31P2-1‑12‑

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35

N. Aizawa, K. Nakamura, H. Akatsu1, T. Abe1, M. Yamanaka2 and C. H. Pyeon2*UDGXDWH6FKRRORI(QJLQHHULQJ7RKRNX8QLYHUVLW\6FKRRORI(QJLQHHULQJ7RKRNX8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 The accelerator-driven system(ADS) has been studied for the transmutation of minor
actinides. Besides, ADS has a potential to be applicable
to a neutron irradiator for an effective production of useful nuclides by providing wide range of neutron energy
from ultrafast to thermal. A neutron spectrum in ADS
core depends on a core structure, a neutron source andneutron multiplication factor. The previous studies havecarried out the measurement of neutron reaction rates forthe activation foils with the threshold of reactions at several MeV energy in the Pb-Bi zoned core [1] and polyethylene (PE) moderated core [2] driven by spallation
neutron source. These results indicated that the effect offast neutrons was increased as subcriticality became
deeper. In the present study, the measurements of reaction
rates for intermediate neutrons were performed throughthe neutron irradiation experiments in ADS with different
three subcriticality level, in order to clarify the effect ofsubcriticality on the reaction rates by intermediate neutrons.
(;3(5,0(176 The ADS experiment was performed
in KUCA A-core combined with spallation neutron
source generated by 100 MeV protons from FFAG accelerator. Figure 1 shows the core configuration. The core
was composed of the PE moderated highly-enriched uranium fuel and the low-enriched uranium mockup fuel.
The activation foils of In, Ta, W and Cu employed in theexperiment are sensitive to intermediate neutrons, andwere set at (M-O, 15). The Au foils set at (O-P, 15) were
for the measurement of thermal neutrons. The foils wereset with and without Cd cover to examine the effect ofthermal neutrons. The experiments were performed with
one critical case and two subcritical cases (0.984 and0.967 in keff) by changing the positions of control rods.
A

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Fig. 1

F(b) Foil with Cd coverFig. 2 Reaction rates of activation foils without Cdcover normalized by Au(n,γ) reaction rate
5()(5(1&(6[1] C. H. Pyeon HWDO, J. Nucl. Sci. Technol.,   (2018)
190-198.
>@ N. Aizawa HW DO, KURNS Progress Report 2018,
PR4-2, (2018)
>@ T. Sato HW DO, J. Nucl. Sci. Technol.,    (2013)913-923.
[4] Y. Nagaya HWDO, JAERI 1348 (2005).

Polyethylene reflector

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Control rod (C3 Partially Inserted)

S

Safety rod (Fully withdrawn)5(68/76 Figure 2 shows the reaction rates of Ta, W
and Cu normalized by the Au(n,γ) reaction rates for threecases. The rates of In were excluded due to insufficientmeasurement accuracy. The reaction rates of bare Ta andCu were increased slightly as subcriticality became deeper. The similar tendencies were observed in the measurement results of foils with Cd cover. The numericalcalculations were also performed for the verification of
the experimental results by the combined use of PHITS[3] and MVP [4]. The C/Es (the ratio of calculation result
to experimental one) were almost the same values regardless of subcriticality, and the calculation results wereconfirmed to coincide with the measurement tendencies.
These results indicated that the subcriticality change had
a possibility to influence not only fast but also intermediate neutron spectrum. The tendency in the W reaction
rates were remained unclear and the detailed analyses
were underway.

Pb-Bi foilCore configuration of KUCA A-core

31P2-2‑13‑

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A. Oizumi1, M. Fukushima1, K. Tsujimoto1,
M. Yamanaka2, and C. H. Pyeon2

ciency of the fission chamber was 0.042 0.002. These
measured value will be used for verification of evaluatednuclear data by conducting detailed analyses.



1XFOHDU6FLHQFHDQG(QJLQHHULQJ&HQWHU-DSDQ$WRPLF
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,QVWLWXWHIRULQWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  To transmute minor actinides(MAs) partitioned from the high-level wastes, the Japan
Atomic Energy Agency has investigated neutronics of theaccelerator-driven system (ADS). In the nuclear transmutation system such as ADS, the nuclear data validation of
MA is required to reduce the uncertainty caused by the nuclear data of MA. To validate the nuclear data, many independent experimental data need to be mutually compared.
An expansion of integral experimental data is the important
issue since there is a limited number of experimental data of
MA. Previously, experiments of measuring fission rate
ratio of neptunium-237 (237Np) and americium-241 (241Am)
to fission rate of uranium-235 (235U) were performed in ahighly-enriched uranium (HEU) core [1, 2]. This study
aims to measure the ratio of the americium-243 (243Am) and235
U fission reaction rates in low-enriched uranium (LEU)
region at the Kyoto University Critical Assembly (KUCA).
(;3(5,0(176  The irradiation experiment of 243Am
and 235U was conducted at A-core in KUCA. Fission reaction rates were measured by using single fission chamber (diameter: 48 mm, height: 120 mm) having a foilsuch as 235U (10 Pg) or 243Am (12 Pg). The simultaneous
measurement of 243Am and 235U fission reaction rates was
conducted at the center voided region surrounded by
LEU rods as shown in Fig. 1. The LEU rod composed of
HEU plates, aluminum (Al) plates, and natural uranium(NU) plates shown in in Fig. 2 has an averaged 235U enrichment of about 17%. The pulse height distributions
from the fission chambers were acquired under the condition of critical core corresponding to a reactor power of
3.5W. The irradiation time was almost 1 hour.
5(68/76  The distributions of pulse height of 243Am
and 235U fission reactions were observed under the critical condition as shown in Fig. 3. The fission reaction
signals need to be separated from noises due to D and J
rays in small pulse height. For example, the fission reaction events of 243Am and 235U in Fig. 3 were determinedby integrating the counts at voltages greater than 0.589
and 0.592, respectively. As a result, the effective total
fission counts of 243Am and 235U were estimated to be
5,208 and 118,664, respectively. Finally, the fission reaction rate ratio of 243Am and 235U was obtained by the total
counts and the number of atoms, and a detection effi-

11

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F

Normal Fuel Rod (1/8"P60

14Partial Fuel Rod (1/8"p16EUEU)

p

Polyethylene moderator

S/ C

Safety or Control Rods

Figure 1. Loaded position of the fission chambers in the
A-core of the KUCA.

HEU (1/16”x 2) NU (1/24”) Al (1/16”x 2)
Polyethylene(10”p+1/2”PEx 17)(18.5”)Al plate Gr (2”)(20.00mm)

Polyethylene(10”p+ 1/2”PEx 20+ 1/4”PE)(20.25”)…

(1/16”HEUx 2+ 1/8”p)x 10(2.5”)(1/16”HEUx 2 + 1/16”Alx 2 + 1/24”NU+ 1/16”Alx 2 + 1/16”HEUx 2)x 20(10.83”)

Reflector (20.5”)(Lower)(1/16”HEUx 2
Gr (2”)+ 1/8”p)x 10 + Void (1.7”)(2.5”)

Fuel (15.83”)(Unit cell 10 + 20 + 10 times)

Reflector (23.95”)(Upper)Figure 2. Schematic drawing of LEU rod in the KUCA-A
core showing in Figure 1.
10000

235U

1000

Counts

243Am

100

10

1
0.0

1.0

2.0

3.0

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Pulse height (V)Figure 3. Fission signals of 243Am and 235U fission
chambers.
5()(5(1&(6>@ C. H. Pyeon, et al., Nucl. Sci. Eng., ,
pp.1023-1032 (2019).
>@ C. H. Pyeon, et al., J. Nucl. Sci. Technol., , 8,
pp.684-689, (2019).

P2-3‑14‑

35

Development of Real-time Subcriticality Monitor
tector, in which small LiF/Eu:CaF2 eutectics scintillators
were dispersed on side surface of a wavelength shifting
fiber. The optical fiber type detector was covered witha 2.5 mm dia. aluminum tube to protect the detection
ele-ment. The PMT signal was digitized and theprocessed in a Field-Programmable Gate Array(FPGA). The in-formation on pulse height, rise timeand detection timing were recorded and transferred toan analysis computer. In the analysis computer, thesedata were processed. Fi-nally, the subcriticality wascalculated in the PC every seconds. The detector
was placed in a core region. The subcriticality waschanged by inserting control and safety rods.
RESULTS: Figure 1 shows the time trends of themeasured neutron count rate and subcriticality measured
by the fabricated subcriticality measurement system.
The estimated prompt neutron decay constantD and area
ratio were consistent with the reactor operation. Although the D and area ratio should not depend on the
count rate, the measured values slightly depend on the
count rate. Figure 2 shows the relation between the ratio of the experimentally estimated parameters and calculated values, E/C, and the detector count rate. The
calculated values were obtained by Monte Carlo simulation with MCNP 6.1. Difference between the estimated
D and area ratio and the calculated values increases withincreasing the count rate. This is because the counting
loss effect causes misestimation in determination of the
subcliticality related parameters. Among three methods,
Rossi-D ,D fitting and area ratio in the pulsed neutron
source (PNS) methods, the D fitting method in the PNS
took less influence compared with other methods. An
error in the a fitting method is evaluated to be within 20%
compared with the simulation values.

K. Watanabe, T. Endo, S. Imai, A. Uritani, A. Yamazaki,
M. Yamanaka1 and C. H. Pyeon1
Graduate School of Engineering, Nagoya University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: The accelerator-driven subcritical(ADS) system has been developed for transmuting minor
actinides and long-lived fission products [1-2]. The
ADS system should keep to be subcritical condition inany case. The subcriticality is desired to be monitored inreal time. We are developing a real-time subcriticality
monitoring system. This system can simultaneously
apply two methods: the PNS and Rossi-D methods, toassure validity of the measured subcriticality. In thisstudy, we performed the subcriticality measurement experiments using the fabricated subcriticality monitoring
system. In addition, we considered the experimental conditions influencing the estimated subcriticality relatedparameters.
EXPERIMENTS: Subcriticality measurements weremade in A-core of Kyoto University Critical Assembly(KUCA). A Pb-Bi target bombarded with 100 MeV
protons from an FFAG proton accelerator, as a pulsed
neutron source. The repetition rate of the pulsed proton
beam was 20Hz. We used a new optical fiber type de-

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2000 4000 6000 8000 10000
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Rossi D
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Area ratio (-U)/Eeff ($)

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REFERENCES:[1] &+3\HRQ-</LP<7DNHPRWRHWDO$QQ
1XFO(QHUJ\  ±

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EU2760

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Time trend of the measured neutron count

10

20
30
40
Count rate (cps)5060Fig. 2Relation between the ratio of the experimentally estimated parameters and calculated values, E/C, and the detector count rate.

rate(top) and the measured subcriticality (bottom).

31P2-5‑15‑

,352-(&75(6($5&+(63URMHFW

‑16‑

35  

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VXUYLYDO   GD\V 

M. Suzuki

3 ,Q WKLV UHVHDUFK LPSRUWDQFH RI FRQWUROOHG,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH .\RWR
8QLYHUVLW\ 

In this research project, twenty two research projects
were included. In this summary, five research projects (P3-5, P3-6, P3-9, P3-10) could not be reported
due to unexpected or uncontrolled events. Details ofeach project is referred to the following contents. Details of each project is referred to the following contents.
3 7KH PDQ\ QRYHOERURQ FRPSRXQGV IURP&KLQD 86 6ZHGHQ DQG 7XUNH\ KDYH EHHQ LQ
YHVWLJDWHG LQ   All of the China boron compound are extremely low toxic and highly watersoluble. Some are excellent and promising B-com for
BNCT
3 In this project, peptide DDS system with A6K
peptide was focused. The new boron delivery systemwith A6K peptide and BSH show new direction ofboron agent in next generation of BNCT.
3 Boron-containing nanoparticle (B-NP) which ispromising for which is promising nanodevice for
BNCT was functionalized with polyglycerol. The resulting B-NP-PG was dispersed in a phosphate buffer
saline (PBS) at very high concentration and the resulting dispersion is very stable for more than one month.
3 The results in this project show that the chicken
egg FKRULRDOODQWRLF PHPEUDQH CAM) model can beused as a reliable model to examine the efficacy of the
BNCT therapy. The CAM tumor can be dramatically decreased by the exposure to a neutron beam. The result
suggest that the CAM model is particularly suited for the
BNCT experiments.
3 In this project, WKHSHSWLGHVHULHV,)%VHULHV
,)%6+DQG,)%3$ QHZO\GHYHORSHGDVDER
URQ GUXJ ZDV LQYHVWLJDWHG XVLQJ WXPRUEHDULQJ
PLFH  Comparing the changes in tumor size in unirradiated tumor models with IF7-BPA and IF7-BSH respectively, it seems that IF7-BPA suppresses tumor growth
relatively.
3 In this project, newly developed LQ YLWUR modelof tumor tissue for BNCT demonstrated the pharmacokinetics of BPA and the efficacy of neutron irradiation by direct observation of Ș -ray/recoiled Li
particle tracks that are corresponding to the distribution of BxPC3 cells.
3 In this project, WKH QRYHO ERURQFRPSRXQG

%$'%  ZDV WHVWHG 7KH FRPELQDWLRQ JURXS RI
VLPXOWDQHRXV XVH RI ERWK %$'% &('  DQG %3$LY  JDYH WKH PRVW VLJQLILFDQW SURORQJDWLRQ RI

3

‑17‑

intracellular locations of boron compounds w a s
s h o w n by the FHOOSHQHWUDWLQJ SHSWLGHV CPP)
conjugation for achieving their sophisticated BNCT
biological activity. This experimental techniques andfindings will contribute to development for BNCT
methodology.
3 In this project, a novel boron compound containing carbon nanostructure like a horn was investigated.
The carbon nanohorns showed better tumor suppression
effect on colony formation test in vitro compared toradiation only group.

3 In this project, a phenylboronic acid
(PBA)-installed polymeric nanoparticle was tested. In
vivo evaluation on a melanoma-bearing mouse model
could reveal that the PBA-NP possesses a highly potent
antitumor efficacy, which could be only provoked byneutron irradiations.
3 ,Q WKLV SURMHFW poly(vinyl alcohol) (PVA)-BPA was tested. 39$%3$ UHYHDOHG WKH HQKDQFHG
LQKLELWLRQ RI WKH WXPRU JURZWKSUREDEO\EHFDXVH
RI WKH KLJKHU LQWUDWXPRUDO %3$ FRQFHQWUDWLRQWKDQ VRUELWRO%3$ GXULQJ WKH WKHUPDO QHXWURQLUUDGLDWLRQ

3 In this project, maleimide-functionalized
FORVR-dodecaborate (MID)- transferrin (TF) conjugates
was investigated regarding to their in vivo selective boron delivery to tumor in colon 26 tumor
bearing mice.
3 A novel boron agent OKD-001 was ef- fective
for BNCT against orthotopic xenograft glioblas- tomamodel. As shown in Fig. 1, OKD-001 plus neutron
irradiation significantly prolong the overall survival ofthe mice in a dose-dependent manner.
3 Pegylated BSH (BAMP) significantly suppressed the tumor growth as compared to other control
groups without remarkable side effect (e.g. weightloss).
3 In this study, oligodeoxynucleotides (ODNs)
bearing hydrophobic and fluorescent BODIPY unit aturidine base (BU) was investigated.as a new boron com-pound.
3,Q WKLV VWXG\ WKH HIIHFWLYHQHVV RI
% 3 $  %1&7 IRU )8 UHVLVWDQFH 26&& LV HYDOXDWHG 3 $UJ*O\$VR 5*' ELQGLQJGdDTPA-incorporated calcium phosphate nanoparticles(Meo) was investigated.as a new boron compound.
35

6FUHHQLQJRIERURQFRPSRXQGIRU%1&7,QWHUQDWLRQDOFROODERUDWLRQVWXGLHV

M. Takagaki and M. Suzuki
/RXLV3DVWHXU&HQWHUIRU0HGLFDO5HVHDUFK,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR
8QLYHUVLW\For the purpose of boron sciences, we havecontinuously screening the many novel boron
compounds mainly for BNCT collaborating with
China, US, Sweden, and Turkey in 2019. Global
paucity of neutron sources is the main reason forinternational demands of collaboration. We
investigated/ screened many compounds mainly for
BNCT for Cancer. We report a brief summary of2019 year.
Materials and Methods.
We already uploaded our standardized experimental
maneuvers on the following URL,
<https://1458ab30-7501-42df-8c2e-ff59d20cecb7.filesusr.com/ugd/ddd07a_cbe194d92fd14397a5db16
90d68a185c.pdf >.
The minimum requirement for our screening
protocol of Boron compound samples (B-com) for
BNCT is water (and/or DMSO)-soluble 30mg forfirst look screening of experiments 1, 2 and 3.
Whole serial steps are as follow.
1. Solubility in a physiological condition
2. Cell toxicity; IC50
3. Cellular BNCT (in-vitro BNCT)
4. Bio-distribution study (neutron induced boron
autoradiography)
5. Animal BNCT (in-vivo BNCT)
6. Pre-clinical study

Fig.1 A summary of in-vitro BNCT effect ofChina B-coms.

Results and Discussion
The figure 1 shows a summary of in-vitro BNCT
effect of China B-coms. All of them are extreamy
low toxic and highly water soluble. Some areexcellent and promising B-com for BNCT andfollowing bio-distribution study of them areinvestigating on the step 4.
The figure 2 is a schematic drawing of tumoricidal
effect of carborane-conjugated anti cancer drug,
MMP inhibitor of USA. The idea of such
conjugation to evaluate synergetic effect isinteresting and exciting. Our data on tumoricidal
effect of carborane conjugated MMP inhibitor
shows MMP inhibitor is fur beyond BNCT effectwithin acceptable dosage.

Fig.2 A schematic drawing of tumoricidal effectof carborane-conjugated anti cancer drug, MMP
inhibitor of USA.

Acknowledgment: This study has been financially
supported by National Research Fund No.
17Ki8536 2017-19 from the Ministry of Education,
Culture, Sports, Science and Technology, Japan.

3

‑18‑

35

7KHVHOIDVVHPEOLQJ$.SHSWLGHQDQRWXEHDV%6+GHOLYHU\V\VWHP
and all culture cells were stained with 0.5% Crystal Violet (CV) in 20% methanol. The colony of CV staining
sample was counted automatically with aCOLyte 3 automatical colony counter machine, (Synbiosis, A Divisionof Synoptics Ltd) and all data was performed statisticalanalysis.

H Michiue, NKondoDQG M Suzuki
1HXWURQ7KHUDS\5HVHDUFK&HQWHU2ND\DPD8QLYHUVLW\-DSDQ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\-DSDQ,1752'8&7,21  In present advanced cancer therapy with surgery, chemotherapy, and radiation therapy,
Glioblastoma multiforme (GBM) is the most treatment-resistant malignant primary brain tumor, with a
median survival of approximately 1.5 year. Therefore,
the development of novel anti-GBM treatment with the
combination of drug and radiotherapy is promising
method of treatment to GBM after surgery, especially for
elderly GBM patients. BNCT is one of the most promising GBM treatment based on the neutron capture andfission reactions occurred by 10B atoms capture with
low-energy neutrons on the irradiation of brain tumor
tissues with thermal or epithermal neutron beams. The
BNCT reaction consists of high energy transfer alphaparticle (4He) and 7Li nuclei with particle range of approximately within the size cell diameter (<10μm).
Recently, the neutron source changed to the accelerator
neutron source that could be installed in hospital fromreactor neutron source. One of the most difficult problem
in BNCT developing has been reported the new boron
drug applied to several malignant tumor except BPA. The
BPA is the leading BNCT boron drug that started fromamino acid analogue fused boron against malignant melanoma. Next, many researcher reported that the system
L-amino acid transporter-1 (LAT-1) expressed in many
malignant tumors. The BSH was used in primary malignant glioma BNCT with the combined usage of BPA. In
that BNCT project, the combination use of BPA and BSH
group showed significantly longer survival outcome
compared to that of single BPA BNCT(;3(5,0(176 All of protocol was administrated in
committee of KURNS. Before 24hr neutron irradiation,
200μM A6K/2mM BSH (final concentration) or 100μM
A6K/1mM BSH (final concentration) was administrated to
U87 deltaEGFR cell line. Just before neutron irradia-tion,
all the cell sample were collected in collecting tube and got
1MW neutron irradiation (thermal neutron flux 1.4X109
neutron/cm2/sec) for 5min (thermal neutron fluence
4.4X1011 neutron/cm2, γ-ray 0.7X10-1 Gy), 15min(thermal neutron fluence 1.1X1012 neutron/cm2, γ-ray
1.7X10-1 Gy) or 30 min (thermal neutron fluence
2.8X1012 neutron/cm2, γ-ray 3.1X10-1 Gy). After irradiation, all glioma cells were re-cultured in 96 well (9×103
cells/well) and checked cell proliferation with Cell Proliferation Reagent WST-1 (Roche, Basel) by microplate
reader (Vient XS, DS Pharma Promo Co., Ltd ) for 48hr.
And colony formation assay was done after 2 weeks culture with U87 delta EGFR in 60 mm culture dish (n=4)

31P3-2‑19‑

5(68/76 As shown in Fig. 1,The boron neutron reaction in vitro with low or high dose A6K/BSH complex
to U87 delta EGFR cells in KURRI: (A) The colony formation assay of U87 delta EGFR with CV staining after 2
weeks of different neutron irradiation time (blue line:
control group, orange line: low dose 100μM A6K/ 1mM
BSH and gray line: high dose of 200μM A6K/ 2mM BSH,
each n=4)

Fig. 1. The boron neutron reaction in vitro with low orhigh dose A6K/BSH complex to U87 delta EGFR cells in
KURRI: the colony formation assay of U87 delta EGFR
(blue line: control group, orange line: low dose 100μM
A6K/ 1mM BSH and gray line: high dose of 200μM
A6K/ 2mM BSH, each n=4) &21&/86,21The boron DDS agent with polymeric macromolecule
DDS such as liposomes,or several boron compounds
were very interesting and expansible tools in preclinical
BNCT experiments. In this time, we focused peptide
DDS system with A6K peptide. In this time, we tried toshow the new boron delivery system with A6K peptide
and BSH, and this would show new direction of boron
agent in next generation of BNCT.

35

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‑20‑

35([DPLQLQJHIILFDF\RIWXPRUPRGHOVIRU%1&7

K. Matsumoto, A. Komatsu, Y. Higashi, Y. Tamari, M.
Suzuki and F. Tamanoi,QVWLWXWHIRU,QWHJUDWHG&HOO0DWHULDO6FLHQFHV,QVWLWXWH
IRU$GYDQFHG6WXG\.\RWR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
Boron Neutron Capture Therapy (BNCT) provides a
promising approach for cancer treatment. While BPA and
BSH have been used as a boron reagent for BNCT, wehave seen development of novel boron agents in the past
years. These include various nano-formulated boron
agents. To evaluate the efficacy of these new agents, it isnecessary to use tumor models. In the past, tissue culture
cells and mouse models have been used. More recently,
tumor spheroids and the CAM (chorioallantoic membrane) assay using fertilized chicken eggs have been developed [1]. We have evaluated the use of these models
for BNCT.
(;3(5,0(176(Exp.1)
Tumor spheroids were prepared by growing GFP labeledovarian cancer cells on a spheroid forming plate for fourteen days. The spheroids were incubated with boron-10
agents which resulted in the distribution of the agentsthroughout the spheroids. The spheroids were exposed toneutron beam at the nuclear reactor for one hour andchanges to the spheroids were examined.
(Exp.2) A similar experiment was carried out with ovarian tumor formed on the CAM membrane of fertilized
chicken eggs. This was prepared by transplanting humanovarian cancer cells onto the CAM membrane. After confirming tumor formation, boron-10 agents were injected
intravenously and the eggs were exposed to neutron at thenuclear reactor for 1 hour. Effect on tumor growth was
examined by observing tumor size as well as by examining tumor weight three days after the exposure.
5(68/76
Exp.1:
Tumor spheroids were formed from human ovarian cancer cells labeled with GFP. They had uniform shape andsize (0.2 x 0.2 mm). Incubation with boron agents such as
BPA-loaded nanoparticle (Rhodamine-B labeled) resulted
in uniform distribution of the agent throughout the spheroids as revealed by the analysis of confocal microscopy.
These spheroids were then irradiated with a neutron beam
for one hour at the nuclear reactor. Two days after the
exposure, the spheroids were examined. The results
showed that little changes have occurred by the neutron
exposure.

P3-4‑21‑

Exp.2:
Three days after transplanting human ovarian cancer cells
onto the CAM membrane, tumor was formed. Boron reagents such as BPA or BPA-loaded nanoparticles were
injected intravenously into the chicken eggs. The amountof boron loaded onto the nanoparticle that was used inthis experiment was examined by ICP-OES. This analysis
revealed the presence of 5.47 ppm of boron in a 10 ml
solution containing 2 mg of nanoparticles, whichamounts to the weight of boron constituting 2.5% of thenanoparticle. The eggs were exposed to neutron beams
for one hour at the nuclear reactor. Two or three days
after the exposure, tumor size and weight were examined.
The results showed that the tumor size was significantly
decreased by the exposure.
&21&/86,21$1')8785(35263(&76
Our results show that the chicken egg CAM model can beused as a reliable model to examine the efficacy of the
BNCT therapy. We have reproducibly demonstrated that
the CAM tumor can be dramatically decreased by the
exposure to a neutron beam. The tumor weight after the
exposure was less than 10 mg while that of the
non-exposure control was around 50 mg. This type ofdramatic effect was not observed with the use of tumor
spheroids. These results suggest that the CAM model isparticularly suited for the BNCT experiments.
In the future, we plan to use the patient-derived chicken
egg tumor model (PDcE model). We have established the
PDcE model by transplanting tumor fragments from theovarian cancer patients as well as by transplanting biopsy
samples from esophageal cancer patients. This will enable testing of the BNCT efficacy with an individual patient tumor.
5()(5(1&(6
1. A. Komatsu, K. Matsumoto, T. Saito, M. Muto, F.
Tamanoi. (2019) Patient Derived Chicken Egg Tumor
Model (PDcE Model): Current Status and Critical Issues.
&HOOV. 10;8(5).

'HYHORSPHQWRIQHZERURQGUXJIRUQH[WJHQHUDWLRQ$%1&7WUHDWPHQW

S. Ishiyama, T.Hatakeyama, S.Yoneyama, C.Oyamaand
M. Suzuki1*UDGXDWH6FKRRORI6FLHQFH+LURDNL8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\,1752'8&7,21  Aomori Prefecture is one of theshortest-lived prefectures in Japan, and the return of shortlived prefectures is a long-cherished desire. Among them,the death rate due to cancer is the highest in both men andwomen nationwide, so it is an urgent task to overcome cancer death as soon as possible. Therefore, in this research,
the aim is to introduce the first BNCT technology in
Aomori Prefecture[1-2] and to develop original technology mainly for (1) A (advanced Aomori) -BNCT and (2)regenerative treatment using artificial tissue after
BNCT[3-4]. In this report, we mainly report on (1) item
mainly on the development of high-performance BNCT
device and animal experiments using newly developed boron drug using this device.
(;3(5,0(176 For animal experiments, the QSC
accelerator and irradiation facility installed by Aomori
Prefecture in 2018 were used as A-BNCT devices. The
peptide series IF7-B series (IF7-BSH and IF7-BPA) newly
developed as a boron drug was administered to tumor
model nude mice (about 80 mice) at a maximum dose of
70 mg / kg by TVI and IP. The irradiation dose was 1.2 ×
1012 n / cm2 and the maximum irradiation time was up to
1 hour.
5(68/76 Fig. 1 shows the tumor volume change of eachtumor model injected with IF7-BPA and IF7-BSH after irradiation with A-BNCT device (indicated by Hot in the
figure), respectively, and unirradiated tumor model (indicated by Cold in the figure).
According to this result, although the variation in tumor
size increases with the passage of irradiation time, in thecase of IF7-BPA, the tumor size rapidly increases 5 days
after irradiation in the non-irradiated tumor model (Cold),
whereas the irradiation(Hot), it can be seen that thegrowth rate in the tumor model is suppressed to someextent.
On the other hand, in the case of IF7-BSH, the tumor
size rapidly increases 6 days after irradiation in theunirradiated tumor model (Cold), whereas the growth ratein the irradi-ated tumor model (Hot) is suppressed tosome extent and it was after 10 days.
Comparing the changes in tumor size in unirradiated tumor models with IF7-BPA and IF7-BSH respectively,
it seems that IF7-BPA suppresses tumor growth relatively.
On the other hand, when comparing the suppressive effect of tumor growth rate with IF7-BPA and IF7-BSH, almost the same suppressive effect is observed, but the time
when the suppressive effect of IF7-BSH appears isslightly later than that of IF7-BPA.

5()(5(1&(6[1] S. Ishiyama, J. of Cancer Therapy, 2014,5,1388-1398.
[2] S. Ishiyama, Y. Imahori, J. Itami and H. Koivunoro, J.
of Cancer Therapy, 2015, 6, 759-766.
[3] S. Ishiyama, Y. Asano, M. Suzuki, M. Akashi and H.
Shimada, J. of Cancer Therapy, 2019, 10, 835-845.
[4] S . Ishiyama and M. Suzuki, J. of Cancer Therapy, 2019,10,1025-1035.
,)%3$
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Fig. 1. Change in tumor volume of tumor seeding model
after IF7-BPA and IF7-BSH dope and irradiation. In the
figure, Cold shows the data of the tumor seeding modelthat was not irradiated after the boron drug administration,and Hot shows the data of the tumor model that was irradiated after the drug administration.

P3-

‑22‑

35

5HVHDUFKDQGGHYHORSPHQWRQQH[WJHQHUDWLRQ$%1&7WUHDWPHQW

S. Ishiyama, T.Hatakeyama, S.Yoneyama, C.Oyamaand
M. Suzuki1*UDGXDWH6FKRRORI6FLHQFH+LURDNL8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\,1752'8&7,21 Aomori Prefecture is one of theshortest-lived prefectures in Japan, and the return of shortlived prefectures is a long-cherished desire. Among them,the death rate due to cancer is the highest in both men andwomen nationwide, so it is an urgent task to overcome cancer death as soon as possible. Therefore, in this research,
the aim is to introduce the first BNCT technology in
Aomori Prefecture[1-2] and to develop original technology mainly for (1) A (advanced Aomori) -BNCT and (2)regenerative treatment using artificial tissue after
BNCT[3-4]. In this report, we mainly report on (2) item
mainly on the development of high-performance BNCT
device and animal experiments using newly developed boron
drug
using
this
device.
(;3(5,0(176
2.1 Cells, reagents and instruments: Normal human dermal-fibroblast (NHDFs) and red fluorescent protein(RFP)-labeled human pancreatic cancer line BxPC3wereused in the experiment. Dulbecco’s modified Eable7s medium (DMEM) containing 10% fetal bovine serum (FBS)
was used to proliferate cells prior to construction of thetumor tissue model. The cells were cultivated at 37Υ, 5%
carbon dioxide. Bovine plasma-derived fibronectin (FN)and porcine skin gelatin(G) were applied in this process.
Cell cultivation were conducted on transwell inserts withporous polyester bottom(pore size: 0.4ȣm) for 12-wellculture plate(12mm diameter, 112mm2 area, cat.
No.3401). 2.2 Preparation of LQ YLWUR human threedimensional tumor tissue model: Human threedimensional tumor was pre-pared by cell accumulation
method. First, connective tis-sue-like structures were
fabricated by three-dimensional lamination of NHDFs. As
shown in Fig.1, NHDFs are cul-tured under the conditions
mentioned above, then ECM-nano film (about 10nm
thick) was formed on each cell sur-face by coating cellswith fibronectin and gelatin dissolved in Tris-HCL buffer.
The cells are seeded on the transwell inserts at a density of
27.2105 cells/insert (8 layers) and cultured under theconditions of 5% carbon dioxide at 37Υ for 12 to 24
hours. We regarded this connective tis-sue-like structure
as an artificial human normal tissue model, termed as
NHDF3D. Next, RFP-labeled BxPC3 cells which havebeen cultured and proliferated were col-lected by trypsin
treatment, washed, and uniformly seeded on the uppersurface of NHDF3D at a density of 300 cells/mm2, thenfurther cultured for 24 hours under the above culture
conditions.
2.3 BPA immersion treatment and fixation: The BPA solution (3%w/v) was diluted to a concentration of 40ppm
with DMEM containing 10% FBS. After removing theculture solution of NHDF3D or NHDF3D/BxPC3, 750
ȣ L of BPA treatment solution was added, and incubatedfor 2 KRXUV %3$H[SRVXUH XQGHUFRQGLWLRQRI

3
‑23‑

carbon dioxide at 37Υ(Fig. 1). After that, the BPA
treatment solution was removed and the tissues were
washed 3 times with 0.01 M phosphate-buffered saline(PBS, PH 7.3). Subse-quently, the tissues were fixed by
4% paraformaldehyde/0.1M phosphate buffer (PH 7.3)
for 30 minutes at room temperature shading the light.
After the fixation, the cellular nucleus was stained by
4’,6-diamidino-2-phenyl-indole(DAPI).
2.4 Neutron irradiation experiment: The above-mentioned
NHDF3D or NHDF3D/BxPC3 in the transwell inserts
were cut out with a knife together with the polyester base,mounted on the solid track detector CR-39 with close
con-tact, and used as a sample for track image acquisition(Fig.1(d)9. Irradiation experiments using these samples were conducted at the heavy water neutron
irradiation facility of Kyoto university reactor(KUR), andirradiation was performed for 30minitues under anirradiation flux of 1.4109 n/cm2/s(Fig.1). After theneutron irradiation, the above sample was etched (6N
NaOH, 70Υ2 hours) to visualize the Ș-ray/recoiled Li
particle tracks generated on the CR-39 surface.
5(68/76 From these results, our LQYLWUR model of tumor tissue for BNCT demonstrated the pharmacokinetics
of BPA and the efficacy of neutron irradiation by direct
observation of Ș-ray/recoiled Li particle tracks that are
corresponding to the distribution of BxPC3 cells. Moreover, the evaluated number of Ș-ray/recoiled Li particle
tracks per single BxPC3 cell or NHDF provide thecompa-rable value with T/N ratio of BPA in the previous
stud-ies[2-3].
5()(5(1&(6>@ S. Ishiyama, J. of Cancer Therapy, 2014,5,1388-1398.
>@ S. Ishiyama, Y. Imahori, J. Itami and H. Koivunoro, J.
of Cancer Therapy, 2015, 6, 759-766.
>@ S. Ishiyama, Y. Asano, M. Suzuki, M. Akashi and H.
Shimada, J. of Cancer Therapy, 2019, 10, 835-845.
>@ S. Ishiyama and M. Suzuki, J. of Cancer Therapy,
2019,10,1025-1035.

Fig. 1 Procedure for detection of BNCT reaction by usingin vitro three-dimensional artificial human tumor tissue
model

35

Evaluation of boron neutron capture therapy (BNCT)
using brain tumor bearing rats or mice model

Y. Fukuo, S. Kawabata, Y. Hattori, H. Kashiwagi,
T. Kanemitsu, K. Takeuchi, R. Hiramatsu, M. Suzuki,SI. Masunaga, H. Nakamura, M. Kirihata, M.Wanibuchi,
S-I. Miyatakegroups (43.4%).

Groupcontrol
Irradiated
BADB control
i.v. BPABADB (CED)
BADB (CED)+ i.v. BPA

Department of Neurosurgery, Osaka Medical College
Laboratory for Chemistry and Life Science, Institute of
Innovative Research, Tokyo Institute of Technology
Institute for Integrated Radiation and Nuclear Science,
Kyoto UniversityOsaka Prefecture University, Research Center of Boron
Neutron Capture Therapy
Kansai BNCT Medical Center, Osaka Medical College

n
6
5
5
6
8
7

Survival TimeMedian Range(95% CI)
26.5
25-28
28
27-29
28
27-29
34
33-36
31
29-34
38
36-39

Table 1. Survival times of F98 glioma-bearing rats after
neutron irradiation

Introduction
Boron neutron capture therapy (BNCT) has been performed as an adjuvant therapy of malignant glioma. We
treated patients with malignant glioma by surgical removal followed by BNCT, and recently reported withgood results.[1]Many new drugs have been proposed to date, but clinical experience is limited to BPA (boronophenylalanine)and BSH (borocaptate sodium).[2] The development ofeffective boron compounds is a major theme. We havebeen conducting the basic study on how the novel boron
compound (BADB) that combines the advantages of using amino acid demand (BPA) and containing a large
amount of 10B per molecule (BSH) for BNCT will affectrat brain tumor model.
Materials and Methods
We used two boron compounds: BPA and BADB. For invivo BNCT study, the therapeutic effect was evaluated interms of the survival time for all rats divided into six
groups: untreated controls, neutron irradiation controls,
non-neutron irradiation with BADB (CED) controls,
BNCT with BPA (i.v.), BNCT with BADB (CED), and
BNCT with combination of BPA (i.v.) and BADB (CED).
The rats were irradiated at a reactor power of 1 MW for 1
hour.
Results
The survival data following BNCT are summarized inTable. 1. Median survival time (MST) in all neutron irradiation groups were significantly longer than that in theuntreated control group (p < 0.005 by Log-rank test, respectively).
The combination group of simultaneous use of both
BADB (CED) and BPA (i.v.) gave the most significant
prolongation of survival (38 (36-39) days). BADB (CED)
and BPA (i.v.) combined group had a significant survival
prolongation compared with the single-agent group. (vs.
BPA (i.v.): 34 (33-36) days, p < 0.05 by Log-rank test, vs.
BADB (CED): 31 (29-34) days, p < 0.05 by Log-ranktest). In addition, the combined group showed the highest
percent increase in life span value (ILS) among all treated

31P3-11‑24‑

Ongoing study
We developed another novel boron drug that humanserum albumin conjugated maleimide-functionalized
closo-dodecaborate (MID-HSA)[3] as 10B carrier for
BNCT. The MID-HSA utilizes the accumulation in thetumor through the well-established Enhanced Permeability and Retention (EPR) effect[4] of solid tumors. We
evaluated the biodistribution of these following BPA,
BSH, and MID-HAS. In biodistribution study, boron uptake in tumor boron concentration was confirmed by intravenous administration of MID-HSA. Blood concentration was high after i.v. administration. In vivo further
therapeutic experiments of MID-HSA using intravenous
and CED as a boron delivery agent are ongoing and theresults will be reported soon.
Reference
 Kawabata S, Miyatake S, Hiramatsu et al (2011) Phase
II clinical study of boron neutron capture therapy
combined with X-ray radiotherapy/temozolomide inpatients
with
newly
diagnosed
glioblastoma
multiforme--study design and current status report.
Applied radiation and isotopes : including data,
instrumentation and methods for use in agriculture,industry and medicine 69 (12):1796-1799.
 Miyatake S, Tamura Y, Kawabata et al (2007) Boron
neutron capture therapy for malignant tumors related tomeningiomas. Neurosurgery 61 (1):82-90.
 Kikuchi S, Suzuki M, Nakamura H et al (2016)
Maleimide-functionalized closo-dodecaborate albumin
conjugates (MID-AC): Unique ligation at cysteine andlysine residues enables efficient boron delivery to tumor
for neutron capture therapy. Journal of controlled
release : official journal of the Controlled Release
Society 237:160-167.
 Matsumura Y, Maeda H (1986) A new concept for
macromolecular therapeutics in cancer chemotherapy:
mechanism of tumoritropic accumulation of proteins andthe antitumor agent smancs. Cancer research 46 (12 Pt
1):6387-6392

35

Intracellular target delivery of cell-penetrating peptide-conjugateddodecaborate for boron neutron capture therapy (BNCT)I. Nakase1,2, M. Katayama1,2, Y. Hattori3, M. Ishimura3, S.
Inaura1, D. Fujiwara1, I. Fujii1, S. Futaki4, and M. Kirihata3
1

Graduate School of Science, Osaka Prefecture University, Japan
2
NanoSquare Research Institute, Osaka Prefecture University, Japan
3
Research Center of BNCT, Osaka Prefecture University,
Japan
4
Institute for Chemical Research, Kyoto University, Japan
Figure 1. Schematic representation of the intracellulartargeted delivery of boron compounds. Boron compounds (dodecaborates, DB) are conjugated to RLA
peptides for mitochondria delivery. The controlled intracellular delivery by the conjugated peptide affects
the efficacy of the cancer cell-killing activity and thecell death types.

INTRODUCTION:In BNCT, internalization of
B-boron atom by cancer cells leads to the induction ofcell death by generation of alpha particles and recoiling
7
Li nuclei with high linear energy transfer and shortrange when irradiated with neutrons [1]. Effective therapeutic benefits on intractable cancer, such as brain tumor
and head and neck cancer have been attained throughcurrent BNCT technology. However, insufficient accumulation and cellular uptake efficacy of second-generation boron compounds such as thiododecaborate (BSH) under clinical research have been pointed out.
In this research, we aim to develop BNCT technology
using cell-penetrating peptides (CPPs) [2] for enhanced
cellular uptake of boron compounds and their controlled
locations inside cells.
10

cluding efficacies and mechanisms) under BNCT. For
example, boron compounds conjugated with mitochondria target CPP, RLA (amino acid sequence:
D[RLARLAR]2) [3], showed significantly enhanced cellular uptake efficacy and mitochondrial accumulation of
the boron compounds (Figure 1). Once the accumulationof the boron compounds in mitochondria (30 min treatment), the compounds were highly retained even after 24
hrs incubation. In BNCT experiments, we found that RLA
peptide-conjugated dodecaborate showed higher effectsof cancer cell-killing activity than that of other CPPs
(endosomes and cytosolic release) when irradiated withneutrons in vitro BNCT assay [4].

EXPERIMENTS: Chemical synthesis of all peptides
were conducted via Fmoc solid-phase peptide synthesis.
Dehydration condensation of carboxyl dodecaborate derivative [B12H11S(CH2)2COOH] to the N-terminal of
CPPs was conducted for their conjugation. Cellular uptake of fluorescently labeled dodecaborate-conjugated
CPPs were assessed using a confocal laser microscopy.
Regarding BNCT assay, after cellular treatment witheach dodecaborate-conjugated CPP (30 min, 37°C), thecells were irradiated with neutrons, and cell-killing effects were detected by e.g. cellular colony assay.

CONCLUSION: In this research, we showed importance of controlled intracellular locations of boron
compounds by the CPP conjugation for achieving their
sophisticated BNCT biological activity. Our experimental
techniques and findings will contribute to developmentfor BNCT methodology.
REFERENCES:>@ K. Nedunchezhian, et al. J. Clin. Diagn. Res. 10(2016) ZE01-ZE04
>@ S. Futaki, I. Nakase, Acc. Chem. Res. 50 (2017)2449-2456
>@ I. Nakase, et al. Chem. Commun. 48 (2012)
11097-11099
>@ I. Nakase, et al. Chem. Commun. 55 (2019)13955-13958

RESULTS: When cell death is induced by organelle
damage, the cell death efficacies and pathways are possibly affected by the damaged organelles (e.g. plasma
membrane, mitochondria, or nucleus) by BNCT. We designed and synthesized organelle-targeted peptide-conjugated boron clusters to increase their cellular
uptake and to control the intracellular locations for induction of sophisticated cancer cell-killing activity (in-31P3-12‑25‑

PR3-9

A novel carbon nanohorns for BNCT
bon nanohorn consists of natural borons, not contains

T. Tsurubuchi1, F. Yoshida1, A. Zaboronok1, K. Nakai1,2,
M. Shirakawa3, Haruka Arita3, Haruna Uto3, M. Suzuki4,
A. Matsumura1

10B. therefore, if we use carbon nanohorns consisting of
10B, we can expect better results the same as BPA or
more.

Graduate School of Science, Kyoto University
1
Department of Neurosurgery, Faculty of Medicine,
University of Tsukuba
2
Department of Radiation Oncology, Faculty of Medicine, University of Tsukuba
3 Department of Pharmaceutical Sciences, University of
Fukuyama
4 Institute for Integrated Radiation and Nuclear science,
Kyoto University

Figure 1

INTRODUCTION:
For Boron Neutron Capture
Therapy ( BNCT ), less toxic and tumor-selective accumulation by ideal drug delivery systems are mandatory.
Many types of newly boron compound such as liposome,porphyrin, and others were developed, none of novel boron compound has been used in BNCT trials other thanp-boronophenylalanine ( BPA ), sodium borocaptate( BSH ). Morever, only BPA proceeded to phase II trial in
the field of BNCT.
We developed a novel boron compound containing
carbon nanostructure like a horn provided by national
institute of advanced industrial science and technology.
This compound contains borons not only inside horn
structure but also the outer surface of this horn. For selective accumulation in tumor cells, the BN-CNH wascoated with phospholipid polyethylene glycol having
folate, BN-CNH/PLPEG-FA [1] called carbon
nanohorns. This carbon nanohorns conjugated with FA
can selectively accumulate in tumor tissues. Also, it canbe observed under light microscope to check whether it isin the tumor tissues and tumor cells [1] .

Figure 2

EXPERIMENTS: CT26, mice colon tumor cells, andGL261, mice glioma cells were used for colony formation test. The 1*106 cells were plated on wells of 6
well plate 24 hours before experiment. The drug, carbon
nanohorns and BPA were added to each well respectively
24 hours before irradiation compared to control, radiation
only group. The cells were trypsinized and counted. The
irradiation was performed with thermal neutrons with aflux of 1.6 x 1012 neutrons/cm2 over 15min at the Kyoto
University Research Reactor (KUR). The 200 cells and600 cells per dish were plated respectively. Plating efficiencies were checked after counting colonies on day 14.
This time carbon nanohorns only contains natural boron.

REFERENCES:[1] Y. Iizumi et al., CARBON 93 (2015) 595-603.

RESULTS: The carbon nanohorns showed better tumor suppression effect on colony formation test in vitro
compared to radiation only group. BPA showed the best
tumor supression effect (Figures 1&2). However, our car-

31P3-13‑26‑

35

                       

A. Kim1, M. Suzuki2, Y. Matsumoto3,4, N. Fukumitsu5,
and Y. Nagasaki1,6,7
'HSDUWPHQWRI0DWHULDOV6FLHQFHV*UDGXDWH6FKRRORI3XUHDQG$S
SOLHG6FLHQFHV8QLYHUVLW\RI7VXNXED,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQ
DQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ )DFXOW\RI0HGLFLQH8QLYHUVLW\RI7VXNXED3URWRQ0HGLFDO5HVHDUFK&HQWHU8QLYHUVLW\RI7VXNXED+RVSLWDO5DGLDWLRQ2QFRORJ\5HVHDUFK/DERUDWRU\'HSDUWPHQWRI
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8QLYHUVLW\RI7VXNXED &HQWHUIRU5HVHDUFKLQ,VRWRSHVDQG(QYLURQ
PHQWDO'\QDPLFV &5L(' 8QLYHUVLW\RI7VXNXED,1752'8&7,21
Boron neutron capture therapy (BNCT) utilizes nuclear
fission in a few Pm-range to achieve target-specific tumoricidal effects. The location of the boron-10 determines
where the nuclear fission takes place, thus the biodistribution of the boron-10 should be regulated to afford damage
in the tumors, but not to provoke adverse effects elsewhere. To this end, we designed a phenylboronic acid
(PBA)-installed polymeric nanoparticle (Fig. 1), of which
tethered PBA moieties provide neutron capture capacity as
well as strong affinity to sialic acids. Because hypersialyation of the cancer cells is generally accompanied bymetastatic invasiveness, the PBA might facilitate accumulation and retention of the nanoparticle, especially inmetastatic tumors. Furthermore, in contrast to conventional BNCT agents, polymeric nanoparticles are notprone to an acute renal clearance, due to a supramolecular
structure comprised of synthetic polymers. Thus, our design is supposed to have a prolonged systemic circulation,
which may result in even higher tumor accumulation.

city assays. In vivo feasibility of the PBA-NP was validated on a B16 melanoma-bearing C57BL6/j mouse model,
by subcutaneous injection of either the PBA-NP or boronophenylalanine-fructose complex (BPA-f), subsequently
irradiated with non-invasive neutrons. Furthermore, microdistribution of the boron-10 could be indirectly monitored by embedding tumor sections on a CR-39 solid state
nuclear track detector, followed by thermal neutron irradiations, then observed with phase contrast microscope.
Pharmacokinetics of the nanoparticles could be validated
by applying an inductively coupled plasma mass spectrometry (ICP-MS) on homogenized tissue samples.
5(68/76Fig. 2. (A) CLSM observation of B16-F10 cancer cell line and
BAOEC primary cells treated with 5 min with rhodamine-labeled
nanoparticles, scale bars represent 20 Pm. (B) Antitumor efficacy of
PBA-NP on BNCT, compared with BPA-fructose (BPA-f), n = 6.

As confirmed by 1H NMR spectra, although the PBA moiety on the synthetic polymer was initially protected withpinacol, it could be readily deprotected while the nanoparticle was being purified, presumably because of hydrolysis-driven deprotection on dialysis. Thus, no further procedure was required to allow functional PBA moieties to be
exposed, and to obtain the PBA-NP. The hydrodynamic
diameter of the PBA-NP was around 75 nm, which was stably sustained under a physiological condition in the presenceof serum, for at least 24 h. With an SPR analysis, the
PBA-NP demonstrated unusually strong and selective binding to a sialic acid-immobilized surface, ensured a targeting
effect. This was consistent with the CLSM observation (Fig.
2A), where brief incubation of the PBA-NP with hypersialyated cancer cell lines clearly showed selective localization
onto the cell membranes. Notably, in vivo evaluation on amelanoma-bearing mouse model could reveal that the
PBA-NP possesses a highly potent antitumor efficacy, which
could be only provoked by neutron irradiations. It is important to state although the PBA-NP was administered at a100-folds lower effective dose (0.24 mg 10B/kg) than that of
the BPA-f (24 mg 10B/kg), their antitumor efficacies on neutron irradiations were comparable to each other (Fig. 2B).
No distinct side effect was observed in the PBA-NP injected
mice, as there was no apparent body weight change in both
irradiated and non-irradiated control groups. Moreover, assured with a series of cytotoxicity assays, none of the normal
primary cells and cancer cell lines manifested palpable response to the PBA-NP. In conclusion, here we propose ahighly efficient BNCT agent which affords an active targeting capability.

Fig. 1. Schematic design of the PBA-installed nanoparticle

(;3(5,0(176Sequential anionic polymerization of ethylene oxide andD,L-lactide was carried out on a PBA pinacol ester bearing
alkoxide initiator, resulted in an amphiphilic copolymer
composed of pinacol-protected PBA, poly(ethylene glycol)(PEG), and poly(lactic acid) (PLA). Subsequently, thePBA-installed polymeric nanoparticle (PBA-NP) was
self-assembled by dissolving aforementioned polymer inan organic solvent, followed by dialysis against distilled
and ion exchanged (DI) water. The PBA-NP was thenevaluated with a series of in vitro analyses, including surface plasmon resonance (SPR) technique, confocal laser
scanning microscopy (CLSM) observations, and cytotoxi-

31P3-14‑27‑

'HVLJQ 6\QWKHVLV DQG (YDOXDWLRQ RI *OXFRVH DQG 0DFURF\FOLF
3RO\DPLQHW\SH %RURQ &DUULHUVIRU%1&7

35

S. Aoki1,2, H. Ueda1, K. Mizuno, C1. Balachandrani1, M.
Suzuki3, S. Masunaga3, N. Kondo3 and Y. Sakurai3

B atoms (fmol/cell)(;3(5,0(176 DQG 5(68/76 The synthesis ofand
carried
out
from
DE
was
D-glucose and D-glucose, respectively.
2-deoxy-2-amino)DFXOW\RI3KDUPDFHXWLFDO6FLHQFHV7RN\R8QLYHUVLW\RI
The synthesis of DH was conducted from the6FLHQFH
1,4-additionof BSH with acrylonitrile and ethyl acrylate,5HVHDUFK,QVWLWXWHIRU6FLHQFHDQG7HKFQRORJ\7RN\R
followedby
the alkylation reaction with 6-TsO deriva8QLYHUVLW\RI6FLHQFH
tives
of
the
1-protected
D-glucosamines (the details will,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
be reported elsewhere). The synthesis of DH was.\RWR8QLYHUVLW\
achieved according to our previous paper [3]. Cytotox,1752'8&7,21  Boron neutron capture therapy icity and cellular uptake activity of the synthesized com(BNCT) is one of powerful therapies for local tumor con- pounds in cancer cells were evaluated by MTT assay andtrol in the treatment of brain tumor, melanoma, and so on ICP-MS (inductivity coupled plasma-mass spectrometer).
[1]. To date, only two boron-containing drugs,
2.0
L-4-boronophenylalanine (BPA) and BSH (sodium
Normoxia
1.8
mercaptoundecahydrododecaborate,
Na2B12H11SH)
Hypoxia
1.6(Fig. 1) have been approved as clinically test compounds,*30 M & 7h incubation for 1, 2a, & 5a,b,e
1.4
and development of better BNCT agents is highly reand 100 M & 24 h incubation for 24 h for 4b,c
1.2
quired.
1.0
0.8
0.6
0.4
0.2
0

)LJ Chemical structures of BSH, BSH, and 
An enhanced uptake of D-glucose and glucose transporter expression are common in cancer cells. In thiscontext, we previously reported on the design and synthesis, of 2-boryl-1,2-dideoxy-D-glucose derivatives (Fig. 1), although its intracellular uptake is not so high[2]. In this paper, we report on new D-glucose-based
drugs DE and  having boryl parts at the C-2 and C-1
positions and DG having BSH unit at the C6 position of
D-glucose and cationic sulfonium unit to neutralize thedianion of BSH part (Fig. 2).
and

OH
O

HO
HO
O

OMe

HO
HO

O

N

R3

O

HO
3 (HU-26)

R2S

2a (HU-17) : -form
2b (HU-18): -form

R2, R3 =

2-

R5

HO
HO

OH
O

S+
O

OH

NHR4
4

4a (KM-3): R = Cbz, R5 = CN
4b (KM-5): R4 = Cbz, R5 = CO2Et
4c (KM-6): R4 = H, R5 = CO2Et
4d (KM-10): R4 = Ac, R5 = CO2Eto-,m-,p-form

OB
O

BPA-D BSH
-flucrosecomplex

1b

2a

4b*

4c*

5a

5b

5e

)LJ  The results of intracellular uptake evaluatoin of
BPA-D-fructose complex, BSH, , DE, EF, and DEH in
HeLa S3 cells, as determined on ICP-MS after the
incubation with 30 PM (for , DE, and DEH) and 100 P
M (for EF) of the drugs under normoxic and hypoxic
conditions at 37 ºC for 7í24 hr. Data represent the mean
±SD of at least three replicates.
The intracellular uptake values of the aforementioned
compounds are presented in Fig. 3, which implies thatthe intracellular uptake of D, E, F, and D is somewhat
better than BPA and BSH. The uptake of E, a zinc(II)complex of D is lower than that of D. The comparisonof D, F (data not shown) and H suggests the potion of
boryl unit on the benzyl groups of these compounds isimportant for the uptake efficiency [4]. The evaluation of
BNCT effect of these molecules and the improvement of
the design of these B-carriers and the attempts at 11B
MRI of these agents are now in progress.
5()(5(1&(6[1] a) R. F. Barth HW DO, &OLQ &DQFHU 5HV,  (2005)
3987-4002. b) R. F. Barth HW DO. 5DG 2QFRO.  (2012)
146-166.
>@ T. Itoh HW DO, %LRRUJ 0HG &KHP.  (2018)5922-5933.
>@ M. Kitamura HW DO ,QRUJ &KHP  (2011)
11568-11580.
[4] H. UedaHWDOUnpublished result.

O
B
O
N n+N HxM
N
H

HN

5a (HU-20): p-form, xMn+ = 2H+
5b (HU-21): p-form, xMn+ = Zn2+
5c (HU-22): m-form, xMn+ = 2H+
5d (HU-23): m-form, xMn+ = Zn2+5e (MK-1): o-form, xMn+ = 2H+)LJ  Structures of boron-containing agents based on
D-glucose and macrocyclic polyamine scaffolds.

31P3-15‑28‑

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5()(5(1&(6* +(4??42HWDO5DGLDW5HV    * + % :8:?:HWDO6FL$GY
0,,E  35'HYHORSPHQWRI&DUULHU3URWHLQEDVHG%RURQ'HOLYHU\6\VWHP

H. Nakamura, S. Kukichi, S. SatoDQGM. Suzuki
/DERUDWRU\ IRU &KHPLVWU\ DQG /LIH 6FLHQFH ,QVWLWXWH RI
,QQRYDWLYH5HVHDUFK7RN\R,QVWLWXWHRI7HFKQRORJ\<RNR
KDPD-DSDQ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 Boron Neutron Capture Therapy(BNCT) of tumor has been focused as one of the minimally invasive cancer therapies. The successful treatmentof BNCT is highly dependent on the sufficient and selective accumulation of 10B atoms to tumor.
We have studied carrier protein-based boron delivery
system. Recently, we developed maleimide-functionalized
FORVR-dodecaborate (MID) [1] aiming to conjugate to serum albumin, as known to accumulate in malignant andinflamed tissues due to the combination of leaky capillaries with the absence or defect of the lymphatic drainage
system, at Cys34 which has only a free SH group among
33 cysteines. Interestingly, MID was found to conjugate
not only to a free SH of cysteine residue but also to lysine
residues in albumin.[2] MID was also conjugated to transferrin (TF), which does not have any free cysteine
residues. TF is an iron carrier protein and accumulated
into cells via TF receptor-mediated endocytosis. It is
known that TF re-ceptor is overexpressed on the surfaceof many tumor cells, thus TF has been used as a ligand
for active targeting in drug delivery system. Herein wereport the preparation of MID-TF conjugates and their invivo selective boron de-livery to tumor in colon 26 tumor
bearing mice.[3]
(;3(5,0(176 MID and isothiocyanate-functionalized FORVR-dodecaborate (ISD) were synthesized from thecommercially available FORVR-dodecaborate triethylammonium form, (Et3NH)2[B12H12] and 10B-enriched FORVR-dodecaborate sodium form, Na2[10B12H12] according to ourpreviously reported procedures.[1] TF was treated with
MID (1.0 mM) or ISD (1.0 mM) in PBS (50 μL) at room
temperature for 1 h. The mixture was subjected to SDSpolyacrylamide gel electrophoresis (PAGE). Immunoblotted with anti-B12H11SH (BSH) antibody was ten carriedout. After further incubation with horseradish peroxidase(HRP)-conjugated secondary antibody, MID-conjugated
TF was visualized with a Molecular Imager ChemiDoc
XRS System. The quantification of MID-conjugated TF
was determined by image analysis program, Image J. Total
proteins (MID-conjugated and unreacted TF) were visualized by coomassie brilliant blue (CBB) staining. Conjugation of MID or ISD to bovine serum albumin (BSA) was
also carried out for comparison.
5(68/76 Figure 1(a) shows the evaluation of the conjugation of MID and ISD to TF. MID and ISD were conjugated to BSA under physiological pH conditions although the conjugation efficacy of ISD was lower than thatof MID against BSA (lane 2 YV 3). Interestingly, ISD similarly conjugated to both BSA and TF even though TF has
no free SH cysteine residue (lane 5 and 6). In our previous

P3-17‑30‑

report, we investigated that MID binds to the lysine residues located in the drug binding sites I and II in albumin.
Based on the observation, efficient conjugation of MID
compared to ISD was probably caused by their different
binding modes in the case of BSA.
We next examined the uptake of MID-TF conjugates bycolon 26 cells which overexpress TF receptors on the cellsurface. The colon 26 cells were incubated with MID-TF
conjugates at 10, 30, and 300 ppm boron concentrationsfor 3 h and the boron accumulation was measured by inductively coupled plasma (ICP). As shown in Figure 1(b),the concentration-dependent uptake of MID-TF conjugates by colon 26 cells was observed. The uptake was not
drastically arrested by addition of TF, indicating that theuptake of MID-TF conjugates is considered to be not only
through the TF receptor mediated mechanism but also
through other pathways.




Fig. 1. (a) Western blot analysis of MID conjugation
to BSA and TF. (b) Concentration-dependent uptakeof MID-TF conjugates by colon 26 cells (black bars).
5()(5(1&(6>@ S. Kikuchi, HWDOJ. Control. Release,  (2016) 160-167.
>@ S. Ishii, HWDOOrg. Biomol. Chem.  (2019)5496 -5499.
>@ S. Kikuchi, HW DO Appl. Radiat. Isotope,  (2020)
109011-109014.

35'HYHORSPHQWRI1RYHO%RURQ$JHQWVIRU%1&7DJDLQVW0DOLJQDQW%UDLQ7XPRUV

A. Fujimura1,2, K. Igawa2, H. Michiue2, A. Ueda2, and
M. Suzuki3*UDGXDWH6FKRRORI0HGLFLQH'HQWLVWU\DQG3KDUPDFHXWLFDO6FLHQFHV'HSDUWPHQWRI3K\VLRORJ\2ND\DPD
8QLYHUVLW\
1HXWURQ7KHUDS\5HVHDUFK&HQWHU2ND\DPD8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Boron neutron capture therapy(BNCT), a well-controlled intracellular atomic reactionof boron 10B, is a cutting-edge cancer therapy. This
QDQRERPE technology utilizes a combination of 10B delivery and neutron irradiation, and consequent 10B nuclear
decay in cell, thus requires high selectivity of 10B delivery into cancer cells for safety and efficacy. Currently,
primary boron agent for BNCT against several kinds ofcancers is BPA (4-borono-L-phenylalanine). BPA is a10
B-added derivative of tyrosine/phenylalanine, and isimported through amino acid transporters such as
LAT1(1). Although LAT1 expression levels are upregulated in almost all cases of head and neck cancers or
melanomas, there are many cases with low expression
levels of LAT1 in the other kind of malignant tumors
including glioblastoma. In these cases, the other types ofboron agents are needed. Our goal of this study is to develop new boron agent for BNCT against malignant brain
tumors, to cover the patients whose LAT1 expression
levels are not high.

Fig. 1. Orthotopic xenograft glioblastoma model mice aretreated with OKD-001-BNCT. OKD-001-BNCT significantly improves the overall survival of the mice in adose-dependent manner.

(;3(5,0(176 NOD-SCID mice were transplantedwith 100,000 cells of patient-derived glioblastoma
stem-like cells MGG8(2) 15 days before BNCT. On 14th
day after transplantation, the mice were injected with 0,
10, 20, 40 mg/kg of OKD-001 (our novel boron agent).
On the next day, these mice were irradiated with neutronfor 1 hour at KUR. After BNCT, the mice were checked
twice a week to draw the overall survival curve. Animal
experiment was approved by the animal experiment ethical committees of Okayama (OKU-2019315) and Kyoto(#17) Universities.

5()(5(1&(6 P. Wongthai et al., “Boronophenylalanine, a borondelivery agent for boron neutron capture therapy, istransported by ATB0,+, LAT1, and LAT2.” Cancer Sci.,
106 (2015) 279-286.
 M.L. Suva et al., “Reconstructing andreprogramming
the tumor-propagating potential ofglioblastoma stem-likecells.” Cell 157 (2014) 580-594.

5(68/76 Our novel boron agent OKD-001 was effective for BNCT against orthotopic xenograft glioblastoma model. As shown in Fig. 1, OKD-001 plus neutron
irradiation significantly prolong the overall survival ofthe mice in a dose-dependent manner.

P3-18‑31‑

35 Experiment on the Anti-tumor Effect of Pegylated BSH by Thermal Neutron Irradiation
M. Shirakawa1,2, N. Kamegawa3, R. Takeuchi3, K. Nakai2,
F. Yoshida2, T. Tsurubuchi2, T. Takata4, M. Suzuki4, A.
Matsumura2 and H. Hori3,51

Department of Pharmaceutical Sciences, University of
Fukuyama
2
Department of Neurosurgery, Faculty of Medicine, University of Tsukuba
3
Morita Pharmaceutical Ind., Ltd.
4
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
5
Niigata University of Pharmacy and Applied Life Sciences
Fig.1) Anti-tumor effect of BNCT by BAMP. (BAMP
24mg10B/kg vs. BAMP 10mg10B/kg : *, vs. BPA
10mg10B/kg : *, vs. BPA 24mg10B/kg : ns, vs. irradiation
only : *, vs. no treatment : ****)INTRODUCTION: Nowadays, novel boron compounds
are frequently demanded to achieve a good anti-tumor
effect. Because, Boron Neutron Capture Therapy (BNCT)
using p-boronophenylalanine (BPA) for carcinoma suchas malignant glioma has a limited therapeutic effect, andthere are many recurrence cases.
Therefore we synthesized novel boron compound
named BAMP [1]. BAMP combined polyethylene glycol(PEG) and mercaptoundecahydrododecaborate (BSH) bycovalent bond. Consequently, pegylated BSH (BAMP)
leads to improvement of blood retention time and accumulation to tumor.
This paper presents the experimental results obtained onanti-tumor effect in vivo using BAMP.
EXPERIMENTS: The tumor-bearing mice were prepared by grafting 5 x 106 of mouse colon carcinoma cells(CT26) to the right thigh of female BALB/cA mice (4weeks old, weighing 16-20 g) to have a tumor diameterof 6-8 mm. These mice were purchased at the age of 3
weeks from CLEA Japan Inc. (Tokyo, Japan) and tamed
in Institute for Integrated Radiation and Nuclear Science,
Kyoto University.
About 11 days after, 200L of BAMP and BPA (as control) were administrated by tail vein injection before irradiation. The dosage was 10mg10B/kg and 24mg10B/kg. At
the interval BAMP was 36 hours and BPA was 2hours,
the irradiation was performed with thermal neutrons witha flux of 1.4-5.9 x 1012 neutrons/cm2 over 1 hour. The
tumor size was measured over time after the irradiation
until Day 24 and calculated using the general formula [2].
Also, a significant difference in tumor size on the lastmeasurement day of each group was calculated by independent t-test. The value of the significant difference andthe number of asterisks are as follows.
(*: p<0.05, ** : p<0.01, *** : p<0.005, **** : p<0.001,
ns: No significant difference)

Fig.2) Body weight of mice after irradiation with the injection of BAMP.

Fig.3) HE stained image of tumor including skin. (A)Image in the BAMP administration group with neutron
irradiation after 24 days. (B)Enlarged image of A (x 40).
(C) Image in neutron irradiation group without administration after 24 days.
REFERENCES:>@ M. Shirakawa, H. Tomida, R. Takeuchi, H. Hori,
Pa-tent applications 2018-156145.
>@ M. Shirakawa, H. Tomida et. al., KURNS PROGRESS REPORT 2018, 55 (2019).

RESULTS: As shown in Fig. 1, Fig. 2 and Fig. 3, BAMP
significantly suppressed the tumor growth as compared toother control groups without remarkable side effect (e.g.
weight loss).

31P3-19‑32‑

35 3UHSDUDWLRQDQG&KDUDFWHUL]DWLRQRI%2',3<7HWKHUHG2OLJRQXFOHRWLGHVIRU%1&7
units from the cells was imaged by means of confocal
microscopy. We observed robust emissions from all cells,
indicating that the aggregates of ODNs were smoothlytransported into cells.

K. Tanabe, M. Suzuki, T. Nishihara and +<DPDVKLWD'HSDUWPHQWRI&KHPLVWU\DQG%LRORJLFDO6FLHQFH&RO
OHJHRI6FLHQFHDQG(QJLQHHULQJ$R\DPD*DNXLQ8QL
YHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 Amphiphilic oligonucleotides withhydrophobic substituents have been widely used as functional materials, and a variety of them have importantfunctions in biological control. For example, modifications of cell membranes, fusion of nanostructures such as
liposomes, and gene manipulations have all been produced by these amphiphilic and functional oligonucleotides.
One of the most useful properties of these amphiphilicoligonucleotides is their aggregate formation that showed
efficient cellular uptake and high level of biological stability within cells. In our recent studies, we demonstrated
the successful delivery of the aggregate consisting ofoligonucleotides into the cells to regulate the gene expression.1
In this study, we prepared oligodeoxynucleotides (ODNs)
bearing hydrophobic and fluorescent BODIPY unit aturidine base (BU). We expected that the ODNs bearing
BODIPY unit would form aggregate to be taken into thecells and express their cytotoxic effect upon irradiation ofthermal neutron. Herein, we synthesize the ODNs andcharacterize their properties.

6FKHPH Synthesis of ODN 1.

(;3(5,0(176&HOOXODU H[SHULPHQWV XVLQJ 2'1V EHDULQJ %2',3<
XQLW ODN 1 (30 PM) were administered to the A549
cells and then the cells were incubated for 23 h. Afterincubation, the cells were irradiated (neutron, 1 MW) for
45 min at KUR. After incubation, WST 8 was added tothe cells, and the cell viability assay was performed using
Microplate Reader.
5(68/76 The synthesis of ODNs bearing BU is outlined in Scheme 1. Phenol group was introduced into
BODIPY unit to give 2, which was alkylated by propargyl bromide under basic conditions. The resulting BODIPY derivative 3 and iododeoxyuridine 5 were coupled by
Sonogashira reaction, and then the silyl groups were removed by treatment with TBAF. The uridine derivative 7(BU) was tritylated and incorporated into DNA via phosphoramidite, using a DNA synthesizer. We prepared 10
mer oligodeoxynucleotides bearing one BU (ODN 1) at
the 5’-end. The structures of ODNs was confirmed by
MALDI-TOF mass spectrometry.
We then conducted cellular experiments with ODN 1
using a human cell line of lung adenocarcinoma, A549.
A549 cells were incubated with the aggregates consistingof ODN 1 at a concentration that was sufficient to form
aggregates, and the fluorescence emission of BODIPY

Based on the above reaction characteristics, an attempt
was also made to demonstrate the radiolytic onset of drug
potency using A549 cells. We investigated the radiation-dependent cytotoxic effect of ODN 1 aggregates.
After administration of ODN 1 aggregates to A549 cells
and incubation for 23 h to allow penetration into the cells,
the cells were exposed to the thermal neutrons for 45 min.
As shown in Figure 1, negligible cytotoxic effect in thepresence of 30 PM ODN 1, was observed. These results
strongly indicate that the concentration of boron atoms in
the cells are not enough to emerge their cytotoxic effects.
Thus, the improvement of the drug delivery method isstill challenging.

)LJXUH  Cytotoxic effect of ODN 1 (30 PM) toward
A549 cells upon thermal neutron irradiation (1 MW, 45
min).
5()(5(1&(6[1] K. Tanabe HWDO, $&6$SSOLHG%LR0DWHULDOV(2019),
4456–4463.

31P3-20‑33‑

35

In vivo HYDOXDWLRQRI%1&7IRU)8UHVLVWDQWRUDOVTXDPRXVFHOOFDUFLQRPD

K. Igawa, K. Tomizawa1, S. Wang2, A. Sasaki2, S.
Ibaraki2, Y. Ichikawa, T. Takata3, M. Suzuki3
1HXWURQ7KHUDS\5HVHDUFK&HQWHU2ND\DPD8QLYHUVLW\)DFXOW\RIOLIHVFLHQFHV.XPDPRWR8QLYHUVLW\*UDGXDWH6FKRRORIPHGLFLQH'HQWLVWU\DQG3KDUPDFHXWLFDO6FLHQFHV2ND\DPD8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The incidence of oral squamouscell carcinoma (OSCC) is increasing gradually with aging
society in Japan. In consideration of the preservation oforgan function, as well as appearance, Boron Neutron
Capture Therapy (BNCT) for head and neck cancer is oneof the effective treatments instead of surgical procedures,radiotherapy, chemotherapy and combined therapy.
OSCC is the most common malignant neoplasm of theoral cavity and has been treated with 5-florouracil (5-FU)
as an anticancer drug. However, the acquisition of resistance to 5-FU is a major problem for successful cancer
treatment. In this study, the effectiveness of BNCT for
5-FU resistance OSCC is evaluated.

Fig. 1. Tumor growth ratio after thermal neutron
irradiation with or without BPA (each group n=5) .

(;3(5,0(176 5-FU resistant oral squamous cell
carcinoma cell line [2] were subcutaneously injected into
the left hind legs of 6-week-old female Balb/c nude mice
(Clea Japan Inc., Japan). Using L-boronophenylalanine(BPA, Katchem, Czech), fructose-BPA complex (200mg/kg) was injected to the tumor bearing mouse before
40 minutes’ irradiation. After neutron irradiation, thebody weight and the diameter of tumor were measured.
The tumor size was calculated according to the following
formula.
Tumor volume [mm3] = (Long diameter [mm]) x (Short
diameter [mm])2 /2
5(68/76 DQG ',6&866,21 As shown in Fig. 1,
BPA group showed significantly decrease in tumor size
compared to non-boron group at 2 weeks after BNCT for
5-FU resistant SCC bearing mice. The mortality of
5-FU resistant SCC bearing mice is 80 % in non-borongroup and 0 % in BPA group.
These results indicate that BNCT is effective to 5-FU
resistant OSCC. Moreover, it is important to validate the
BNCT for cisplatin resistant OSCC [3]. In near future,
the multidisciplinary approach including BNCT is proposed for refractory OSCC.

31P3-21‑34‑

5()(5(1&(6>@Kato I, Fujita Y, Maruhashi A et al. Effectiveness ofboron neutron capture therapy for recurrent head andneck malignancies. Appl Radiat Isot 67(Suppl.):S37–S42,
2009>@Harada K, Ferdous T and Uneyama Y. Establishmentof 5-fluorouracil-resistant oral squamous cell carcinoma
cell lines with epithelial to mesenchymal transitionchanges International Journal of Oncology 44: 1302-1308,
2014>@Miyazaki H, Takahashi R, Vila M et al. CD44 exerts afunctional role during EMT induction in cisplatinresistanthead and neck cancer cells Oncotarget, Vol. 9, (No. 11),
pp: 10029-10041, 2018

35 $QWLWXPRUHYXOXDWLRQRI*DGROLQLXP1HXWURQ&DSWXUH7KHUDS\WKURXJKFRPSDULVRQRIWXPRUVL]HXVLQJ*G'73$LQFRUSRUDWHGFDOFLXPSKRVSKDWHQDQRSDUWLFOHV
the possibility of RGD sequence binding Meo nanomicellefor clinical applications of NCT.

+ ;XDQ+<DQDJLH0<DQDJDZD
< 6DNXUDL.0RXUL1'HZL+&DEUDO
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0 6X]XNL60DVXQDJDDQG+7DNDKDVKL


'HSWRI1XFOHDU(QJLQHHULQJ 0DQDJHPHQW6FKRRORI(QJLQHHULQJ 8QLY RI 7RN\R 'HSW RI %LRHQJLQHHULQJ
6FKRRORI(QJLQHHULQJ8QLYRI7RN\R &RRSHUDWLYH8QLW
RI0HGLFLQH (QJLQHHULQJ8QLYRI7RN\R+RVSLWDO 1LL
JDWD8QLYRI3KDUPDF\ $SSOLHG/LIH6FLHQFHV2ELKLUR
8QLYRI$JULFXOWXUHDQG9HWHULQDU\0HGLFLQH2VDND&LW\
8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ .\RWR8QLY,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQ 1XFOHDU6FLHQFH
ZLWKLUUDGLDWLRQ /HIW   ZLWKRXWLUUDGLDWLRQ 5LJKW 
5*'JURXS

,1752'8&7,21In our previous report, the anti-tumor effect of GdDTPA-incorporated calcium phosphate nanoparticles(Meo) was improved, and it had the possibility to be applied to the intensive cancer treatment in the future [1,2,3].
However, although the Gd-DTPA-incorporated calcium
phosphate nanoparticle can bind tumor tissues through the
EPR pathway, considering to improve the tumor targeting
ability and drug accumulation in tumor, we introduced
Arg-Gly-Aso(RGD), which is a peptides that can target

many kinds of cancer cells through the integrin.
In this work, we checked the antitumor effect of this material again and focused on the change of the tumor size.
We took the photos at the 30st day after irradiation to compare the antitumor effect of each samples.

ZLWKLUUDGLDWLRQ /HIW ZLWKRXWLUUDGLDWLRQ 5LJKW 
0HRJURXS

(;3(5,0(176
Tumor-bearing mouse models were developed with colon 26 tumor cells and after synthesis of Meo and RGD
binding Meo, they were injected into mice, respectively.
At the 24h after administration, these mice received
thermal neutron irradiation at Nuclear Reactor Facility of
Kyoto Univ Institute for Integrated Radiation & Nuclear
Science with average neutron fluence of 2.0 × 1012 n/cm2.
Moreover, considering the influence of neutron, the same
samples were also injected into mice but without irradiation.
After almost one-month observation, the situation of allmice was recorded and the conclusion about antitumor effect was showed below according to the tumor size comparison photos.

ZLWKLUUDGLDWLRQ /HIW ZLWKRXWLUUDGLDWLRQ 5LJKW &RQWUROJURXS)LJXUH 7XPRU JURZWK VXSSUHVVLRQ E\ *G1&7
XVLQJ5*'0HR0HRQDQRPLFHOOH

5(68/76
In this experiment, tumor growth was suppressed in thegroups of RGD sequence binding Meo nanomicelle and
Meo nanomicelle compared with the non-irradiated groups
with the injection of same DDS. In this time,the tumour
decresence by RGD nanomicelle and Meo nanomicelle
was almost same effect by NCT.
We will check the expression of integrin receptors inColon 26 cancer cell line, and evaluate the uptake of Gd
atoms in the cancer cells by endocytosis. We also evaluate

5()(5(1&(6>@ Dewi N et al., Biomed & Pharmacother (2013) :451-7.
>@ Dewi N et al., J Can.Res.Clin.Oncol. (2016) (4):767-75.
>@ Mi P et al.: J Cont. Release (2014) :63-71.

31P3-22‑35‑

,352-(&75(6($5&+(63URMHFW

‑36‑

35

&OLQLFDOUHVHDUFKRQH[SORUDWLRQVLQWRQHZDSSOLFDWLRQRI%1&7

M. SuzukiDQG H Yanagie1,2,3,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH .\RWR
8QLYHUVLW\

,QVWLWXWHRI(QJLQHHULQJ,QQRYDWLRQ6FKRRORI(QJLQHHU
LQJ7KH8QLYHUVLW\RI7RN\R&RRSHUDWLYH 8QLW RI 0HGLFLQH
8QLYHUVLW\RI7RN\R+RVSLWDO

porous glass (SPG) membrane to the preparation of
BSH-entrapped WOW emulsion for clinical use. De-

10 (QJLQHHULQJ 7KH

5HVHDUFK,QVWLWXWHRI+HDOWK\/LYLQJ1LLJDWD8QLYHUVLW\
RI3KDUPDF\ $SSOLHG/LIH6FLHQFHVAn accelerator-based boron neutron capture therapy(BNCT) system and boronophenylalanine (BPA)-based
new drug were approved by the Ministry of Health, Labour and Welfare of Japan for the treatment of locallyunresectable recurrent or unresectable advanced headand neck cancer on March 2020. Since BNCT will be
carried out at the medical institute, the accessibility of
BNCT will improve dramatically and much greater patients will be treated with accelerator-BNCT comparedwith reactor-BNCT.
In 2019, under the Low on Clinical research* (rinsho
kenkyu hou), clinical researches on BNCT for local recurrent breast cancer and angiosarcoma have been approved.
*/DZRQ&OLQLFDOUHVHDUFK rinsho kenkyu hou New
regulation on clinical research, Law on clinicalResearch (ULQVKR NHQN\X KRX), has come into effectsince April in 2018. Clinical researches conducted byusing Drugs and Medical Devices not approved under
the Pharmaceutical and Medical Device LAW are categorized into Specified Clinical Research (WRNXWHLULQVKR
NHQN\X). Specified Clinical Research Plan should be
reviewed by Certified Clinical Research Review Committee. Since BNCT is carried out using unapproved
drug (boron compound) and research reactor, BNCT
study is categorized into Specific Clinical Research. Six
clinical researches on BNCT have been approved asSpecific Clinical Research by Certified Clinical Research Review Committee established in medical institutes.
In this research projects, two researches are included.
3 We treated one patient suffering from angiosarcoma of the face in this research program. Since thepatient treated with BNCT in this research problem areunder-observation, no detailed report is available.
3
No patient was enrolled in this clinicalresearch program. Yanagie et al. reported a preclinicalstudy on syringe-shaped medical device attached with
Shirasu

3

‑37‑

tails in this case report is referred to the P4-2 report.

35&OLQLFDOUHVHDUFKRQH[SORUDWLRQVLQWRQHZDSSOLFDWLRQRI%1&7

M. Suzuki, M. Iwamoto1, J. Sugawara2, S. Moriwaki3, H.
Tanizaki3 K. Yoshida4, S. Kawabata5, S. Miyatade6, S.
Masunaga, Y. Kinashi, H. Tanaka, Y. Sakurai, N. Kondo,
Y. Tamari, T. Fujimoto7,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR
8QLYHUVLW\'HSDUWPHQWRI%UHDVWDQGHQGRFULQHVXUJHU\2VDND0HGLFDO&ROODJH
'HSDUWPHQWRI2SKWKDOPRORJ\2VDND0HGLFDO&ROODJH
'HSDUWHPHQWRIGHUPDWRORJ\2VDND0HGLFDO&ROOHJH'HSDUWPHQWRI5DGLRORJ\2VDND0HGLFDO&ROOHJH'HSDUWPHQWRI1HXURVXUJHU\2VDND0HGLFDO&ROOHJH
&DQFHUFHQWHU2VDND0HGLFDO&ROOHJH'HSDUWPHQWRI2UWKRSHGLF6XUJHU\+\RJR&DQFHU&HQWHU

An accelerator-based boron neutron capture therapy(BNCT) system and boronophenylalanine (BPA)-based
new drug were approved by the Ministry of Health, Labourand Welfare of Japan for the treatment of locally unresectable recurrent or unresectable advanced head and neckcancer on March 2020. Since BNCT will be carried out
at the medical institute, the accessibility of BNCT will improve dramatically and much greater patients will betreated with accelerator-BNCT compared with reactorBNCT. One of the drawbacks of BNCT is that thermal
neutrons necessary for tumor control cannot be delivered
to the deep portion of the tumor which is located at > 6 cm
in depth from the skin surface.
For BNCT to be recognized as effective treatment modality for malignant tumor, expanding indication of BNCT
is very important.

We treated one patient suffering from angiosarcomaof the face in this research program. Since the patient
treated with BNCT in this research problem are underobservation, no detailed report is available.

3

‑38‑

35

3UHSDUDWLRQRI%RURQHQWUDSSHG:2:HPXOVLRQE\0L[LQJ0HGLFDO'HYLFH
IRU%RURQ1HXWURQ&DSWXUH7KHUDS\WR+HSDWRFHOOXODU&DUFLQRPD

Hironobu Yanagie1,2,3, Mitsuteru Fujihara4, Ryouji
Mizumachi5, Yuji Murata5, Yuriko Sakurai1,2,3, Atsuko
Shinohara6,7, Takehisa Matsukawa7, Ayano Kubota7,
Yasuyuki Morishita8, Novriana Dewi3, Masashi
Yanagawa9, Kazuhito Yokoyama7, Shushi Higashi10,
Kouji Seguchi10, Ichiro Ikushima11, Yoshinori Sakurai12,
Hiroki Tanaka12, Minoru Suzuki12, Shinichiro
Masunaga12, Koji Ono13, Minoru Ono2,14, Jun
Nakajima2,15, and Hiroyuki Takahashi1,2saline solution and surfactant through a second SPG controlled pore glass membrane using this medical device.
The 10B concentration in WOW vesicles was determined
by ICP-AES of Jyuntendo University.
5(68/76 By using this device, we were able to produce the WOW emulsion of the same size even after
changing the persons who perform the experiment morethan ten times. About 7300 ppm 10B concentrations wererecognized in the 10BSH-WOW emulsion as same as Day
0 and Day 1 after preparation using Mixing medical device (Table 1).
In the conventional preparation of WOW emulsion, theprocedure takes about 6 hours. By using this device, wewere able to prepare the WOW emulsion with the single
peak of 100 μm in about 30 minutes.
Since WOW emulsion can deliver high amounts of 10B
to tumor as the first targeting delivery to tumor. We hope
to develop the second targeting delivery to cancer cellswith the increase of mechanism by endocytosis, fusion,
etc.

1Institute of Engineering Innovation, School of Engineering, The University of Tokyo, 2Cooperative Unit ofMedicine & Engineering, The University of Tokyo
Hospital, 3Research Institute of Healthy Living, Niigata
University of Pharmacy & Applied Life Sciences, 4SPG
Techno Ltd. Co., 5LSI Medience Ltd Co, 6The Graduate
School of Seisen University, 7Jyuntendo University,
8
Dept. of Human & Molecular Pathology, Graduate
School of Medicine, The University of Tokyo,
9
Veterinary Medical Center, Obihiro University ofAgriculture & Veterinary Medicine, 10Dept. of Surgery,
Kojin-kai Medical City East Hospital, 11Dept. of Radiology, Miyakonojo Meteropolitan Hospital, 12 Kyoto Univ.
Institute for Integrated Radiation & Nuclear Science,
13
Kansai BNCT Medical Center, Osaka Medical College,
14
Dept. of Cardiac Surgery, The University of Tokyo
Hospital, 15Dept. of Pulmonary Surgery, The Universityof Tokyo Hospital, JAPAN.

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 
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 
 
 
 0HDQ
6',1752'8&7,21  Hepatocellular carcinoma (HCC)
is one of the difficult cancers to cure with conventional
treatment. Higashi et al prepared a long term inseparable
Water-in-oil-in-water(WOW) emulsion for use in arterial
injection therapy to treat patients with HCC by the double
emulcificating technique[1]. Suzuki et al. had reported
the tumor growth suppression by BNCT using boron
compound with IPSO administered intra-arterially[2]. We
performed preclinical BNCT study using 10BSH entrapped WOW [3], and had experienced clinical BNCT
study for HCC using this system[4].
In this study, we developed syringe-shaped medical
device attached with Shirasu porous glass (SPG) membrane to the preparation of 10BSH-entrapped WOW
emulsion for clinical use, and evaluated the boron encapsulating activity to measure the 10B concentrations ofWOW emulsion by using ICP-Mas.

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


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                     


7KH RULJLQDO % FRQFHQWUDWLRQ SSP  LQ :2: HPXOVLRQZDVGHWHUPLQHGXVLQJ,&3$(6DW-XQWHQGR8QLYHUVLW\

5()(5(1&(6>@ S Higashi S HWDO, Cancer, (1995):1245–1254.
>@ M SuzukiHWDO, Jpn J Clin Oncol. 37(2007):376- 81.
>@ H Yanagie HWDO, Br J Radiol.,doi: 10.1259/bjr.
20170004
>@ H Yanagie HWDO, Appl Radiat Isot., (2014):32-7.

(;3(5,0(176 We developed the syringe-shaped
medical device by attaching to SPG Millipore membrane.
10
BSH (262.5 mg) was dissolved in 1.5 ml of a 5% glucose solution, which was first filtered through an SPG
controlled pore glass membrane and then emulsified in
1.5 ml IPSO containing surfactant to form the water-in-oil emulsion (WO). The WO emulsion was thenemulsified again with an aqueous phase containing 3 ml3

‑39‑

,352-(&75(6($5&+(63URMHFW

‑40‑

35

(VWDEOLVKPHQWRI,QWHJUDWHG6\VWHPIRU'RVH(VWLPDWLRQLQ%1&7

Y. Sakurai,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\%$&.*5281'6$1'385326(6There are a number of subjects, which should be improved for the further advance and generalization of boron neutron capture therapy (BNCT). In the viewpoints ofmedical physics and engineering, the advance for dose
estimation is one of the important subjects. The purposesof this project research are the advance for various dose
estimation methods, and the establishment of an integrated system for dose estimation in BNCT.
In the third year of this research project, 2019, the advancement for the respective dose estimation methods
were forwarded mainly using Heavy Water Neutron Irradiation Facility (HWNIF) and E-3 Neutron Guide Tube
(E-3) at KUR, sequentially the previous year. In addition,
the integrated system was considered for the simultaneous usage of several dose estimation methods.
5(6($5&+68%-(&76
The collaboration and allotted research subjects (ARS)
were organized as follows;$56 3  Establishment of characterization estimation method in BNCT irradiation field using Bonner
sphere and ionization chamber (III). (Y. Sakurai, S. Shiraishi, N. Matsubayashi, K. Okazaki, A. Sasaki, Y.
Kumagai, T. Naito, T. Nakamura, Y. Kakimoto, H.
Matsunaga, T. Takata and H. Tanaka)$56 3  Study on new type of neutron spectrometer for BNCT. (A. Uritani, A. Ishikawa, K.
Watanabe, S. Yoshihashi, A. Yamazaki and Y. Sakurai1)$56 3  Neutron measurement by using theself-activation of iodine-added plastic scintillators. (A.
Nohtomi, Y. Hanada, G. Wakabayashi, Y. Sakurai and T.
Takata)$56 3  Characterization of active neutron
detector for boron neutron capture therapy. (M. Takada,
S. Endo, H. Tanaka, T. Matsumoto, A. Masuda, T.
Nunomiya, K. Aoyama and T. Nakamura)$56 3  Study for microdosimetry using silicon-on-insulator microdosimeter in the BNCT irradiation field (III). (Y. Sakurai, N. Ko, T. Takata, H. Tanaka,
T. L. Tran, J. Davis, S. Guatelli, A. Rozenfeld, N. Kondo and M. Suzuki)$56 3  Measurement of BNCT beam component fluence with polymer gel detector. (K. Tanaka, Y.
Sakurai, T. Kajimoto, Y. Ito, H. Tanaka, T. Takata and S.
Endo)$56 3  Development of neutron fluence distribution measuring device using Thermoluminescenceslabs. (K. Shinsho, R. Oh, M. Tanaka, S. Yanagisawa, H.
Tanaka, T. Takata, G. Wakabayashi and Y. Koba)$56 3  The study for development and appli-

31P5

‑41‑

cation of tissue equivalent neutron dosimeter. (M. Oita,
T. Kamomae, T. Takada and Y. Sakurai)$56 3  Development and evaluation of 3D
gel dosimeter for the measurement of dose distributionin BNCT. (S. Hayashi, Y. Sakurai, M. Suzuki and T.
Takata)$56 3  Establishment of beam-quality estimation method in BNCT irradiation field using dual
phantom technique (III). (Y. Sakurai, T. Takata, H.
Tanaka, N. Kondo and M. Suzuki)$56 3  Characteristics test of a prompt
gamma-ray detector using LaBr3(Ce) scintillator and
8×8 array MPPC for boron neutron capture therapy. (K.
Okazaki, K. Akabori1, T. Takata, S. Kawabata, Y. Sakurai and H. Tanaka)$56 3  Developmentof fiber-reading radiation monitoring system with a red/infrared-emitting
scintillator at 60Co radiation facilities. (S. Kurosawa, S.
Kodama, T. Takada, Y. Sakurai and H. Tanaka)$56 3  Establishment of the imaging
technology of 478 keV prompt gamma-rays of boron-neutron capture reaction and the measurementof the intensity of the neutron field. (T. Mizumoto,
S. Komura, Y. Sakurai, A. Takada, T. Takata and T.
Tanimori)$56 3  Feasibility study of a gel-dosimeter
for a quality assurance and a quality control in boron
neutron capture therapy. (S. Nakamura, K. Iijima, M.
Takemori, H. Nakayama, S. Nishioka, H. Okamoto, Y.
Sakurai, H. Tanaka, T. Takata, M. Suzuki, H. Igaki and
J. Itami)$56 3  Optimization of bolus shape for boron neutron capture therapy using epi-thermal neutron
beam. (T. Takata, H. Tanaka, A. Sasaki, Y. Sakurai, A.
Maruhashi and M. Suzuki)$56 3  Development of novel radiochromicgels for assessing 3-dimensional dose distribution inbrain. (H. Yasuda, J.E. Tano, C.A.B. Gonzales and Y.
Sakurai)$56 3  Measurement of neutron distributions in the BNCT irradiation field using a GEM detector. (S. Uno, T. Koike, K. Miyamoto, K. Nobori and H.
Tanaka)$56 3  Development of epi-thermal neutron
flux intensity detector for BNCT. (I. Murata, K. Aoki, Y.
Miyaji, S. Kusaka, H. Tanaka, Y. Sakurai and T. Takada)$56 3  Investigation of thermal neutron-induced soft errors in semiconductor devices. (H.
Tanaka, T. Kato, H. Matsuyama, T. Takata and Y. Sakurai)
For ARS-3, no results were obtained because the insufficient neutron intensities of HWNIF for this subject. For
ARS-19, the animal experiments at E-3 were originallyplanned but could not be performed, because the registration of E-3 as an animal experimental room was not intime. So, the reports of these subjects are not appeared.

35

(VWDEOLVKPHQWRIFKDUDFWHUL]DWLRQHVWLPDWLRQPHWKRGLQ%1&7LUUDGLDWLRQILHOGXVLQJ%RQQHUVSKHUHDQGLRQL]DWLRQFKDPEHU ,,, 

Y. Sakurai, S. Shiraishi1, N. Matsubayashi1, K. Okazaki1,
A. Sasaki1, Y. Kumagai1, T. Naito1, T. Nakamura1, Y. Kakimoto1, H. Matsunaga1, T. Takata, H. Tanaka

Independence Selection (HIS) [5].
On the assumption of the application in the standard
epi-thermal neutron irradiation mode of KUR-HWNIF,
the combination of the moderators for boron-10 concentration and diameter was optimized by HIS. Based on thisoptimization, a configuration of an RBS was decided anda prototype of RBS was made. An experiment was performed for the characteristic verification of the prototype
RBS in the standard epi-thermal neutron irradiation modeof KUR-HWNIF.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\2VDND0HGLFDO6FKRRO,1752'8&7,21  Research and development into
several types of accelerator-based irradiation systems forboron neutron capture therapy (BNCT) is underway [1,2].
In the near future, BNCT using these newly developed
irradiation systems may be carried out at multiple facilities across the world. Considering this situation, it is important that the estimations for dose quantity and quality
are performed consistently among several irradiation
fields, and that the equivalency of BNCT is guaranteed,within and across BNCT systems. Then, we are establishing the quality assurance and quality control (QA/QC)
system for BNCT irradiation field.
As part of the QA/QC system, we are developing estimation method for neutron energy spectrum using Bonner
sphere [3]. For our spectrometer using Bonner sphere,liquid such as pure water and/or boric acid solution isused as the moderator. A multi-layer concentric-spherecase with several sphere shells is prepared. The moderator and its diameter are changeable without entering theirradiation room, by the remote supply and drainage ofliquid moderator in the several layers. For the detector,
activation foils are remotely changed, or online measurement is performed using SOF (scintillator with opticalfiber) detector containing boron, etc. [4].
In 2019, a prototype of the Remote-changeable Bonner-sphere Spectrometer (RBS) was made. An experiment was performed for the characteristic verification of
the prototype RBS at Heavy Water Neutron Irradiation
Facility of Kyoto University Reactor (KUR-HWNIF).

5(68/76 The configuration of the RBS was decided
as follows. A five-layer concentric spherical acrylic shellis used as a container. Each acrylic wall is 1 mm inthickness. The moderator injection part is 9 mm in thickness for each layer. Pure water and 0.15-weight-percent
boric acid water for boron-10 (45 g/Ɛ solubility for
H3BO3 at 20 degree Centigrade) were used as liquid
moderators. A LiCaF scintillation detector is used.
Figure 1 shows an example of the optimized combinationof moderator injection patterns for RBS. Photo 1 shows aprototype RBS, which was made based on the optimization. It was confirmed that the experimental results werein good agreement with the simulation results for the ratios of the detector responses for the respective moderator
injection patterns.
&21&/86,21 We plan to further analyze the experimental data, and improve the prototype RBS.

Fig. 1. An example of the optimized combination ofmoderator injection patterns for RBS.

0(7+2'6 In the neutron energy spectrometry by
Bonner-sphere, the combinations of the moderator material and diameter should be previously decided and prepared. Of course, the more information can be obtained
as the more moderators and detectors are prepared.
However, the information number from those measured
data is less than the combination number, because of theoverlapped regions among the combinations. The selection is important, in which the more information number
is obtained for the combination number.
The combination of moderator and detector is decided,
for that the response functions cannot be approximatedby the linear functions of the other response functions.
The accuracy and precision for the spectrometry can behigher, because the independent information can be obtained from the measurement by the respective combinations. We were developed the selection method, High

Photo 1. A prototype RBS.
5()(5(1&(6[1] H. Tanaka HW DO, Nucl. Instr. Meth. B  (2009)
1970-1977.
[2] H. Kumada HW DO, Appl. Radiat. Isot.  (2014)211-215.
[3] H. Ueda HWDO, Appl. Radiat. Isot.  (2015) 25-28.
[4] M. Ishikawa HW DO, Radiat. Oncol.  (2016)
105(1-10).
[5] H. Ueda, Doctoral Thesis (2016).

31P5-1‑42‑

Study on New Type of Neutron Spctrometer for BNCT35A. Uritani, A. Ishikawa, K. Watanabe, S. Yoshihashi, A.
Yamazaki and Y. Sakurai1

ricated detector was irradiated with intense neutrons withthe flux of 4x108 n/cm2/s at Heavy Water Irradiation Facility of Kyoto University Reactor.

Graduate School of Engineering, Nagoya University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University

RESULTS: Figure 1 shows pulse height spectrum obtained from the fabricated optical fiber type detector using the Li glass scintillator. The detector shows a clear
neutron peak. This is because a high NA optical fiber isused in the detector. The high NA optical fiber helps toefficiently collect scintillation photons from low lightyield scintillator.
Figure 2 shows the time trend of the neutron peakchannel during irradiation with intense neutrons with theflux of 4x108 n/cm2/s. No significant deterioration of
the signal gain was confirmed. Since the fabricateddetector used the silica fiber, the detector is considered toshow sufficient radiation hardness.

INTRODUCTION: Boron neutron capture therapy(BNCT) is a promising treatment method for cancers
such as brain tumors. Recently, an accelerator-driven
neutron source has actively been developed owing to its
simplicity of management. In commissioning phase of
the facilities, specifications of the irradiation field, suchas neutron intensity, the neutron energy spectrum andgamma-ray contamination, should be characterized inorder to assure designed ones.
We are developing a new neutron energy spectrometerusing the optical fiber type detector. The conventional
technique for neutron spectrometry is the Bonner sphere
method. Generally, moderation based neutron spectrometers should be improved in energy response especially for epi-thermal neutron energy region. In order toimprove the energy response, the number of detectors
with different responses should be increased. We proposes the spectrometer consisting of liquid moderator andthermal neutron flux profile scanner using the opticalfiber type detector. So far, we has developed the opticalfiber type detector showing a neutron peak in the pulse
height spectrum [1]. The detector used the Eu:LiCaAlF6
scintillator, which has relatively slow decay time of 1.6
Ps. In order to expand the dynamic range of the neutron
detector, it is desired to use faster scintillator to improvethe counting rate capability. As a fast neutron scintillator, the Li glass scintillator is well known. However, thelight yield of the Li glass is quite low compared with the
Eu:LiCaAlF6 scintillator. Therefore, it was considered
to be difficult to fabricate the optical fiber type detector
showing a neutron peak.

REFERENCES:[1] K. Watanabe et al., Nuclear Instruments and Methods in Physics Research Section A , 802, 1 (2015)

800

Count [a.u.]

600

~2mmΦ

UV curable resin
Heat shrinkage tube

Heat shrinkage tube

Heat shrinkage tube

Optical fiber

Jacket

200
500
1000
1500
Channel number [ch]2000

Fig. 2 Pulse height spectrum obtained from the opticalfiber neutron detector using the Li glass scintillator.

Channel number ofchannelthe Peakneutronpeak[ch][ch]Li-glass
Li-

CarbonReflective coating

400

0
0

EXPERIMENTS: We fabricated the optical fiber typeneutron detector using Li glass scintillator. A small
piece of the Li glass scintillator was mounted at a tip of
the optical fiber. The scintillator was coated with a reflector powder and then covered with a heat shrinking
tube for light shielding. Figure 1 shows the fabrication
procedure of the optical fiber type detector using the Liglass scintillator.
Core & cladding

Shutter
neutronOpen
background
Close

Fig. 1 Fabrication procedure of the optical fiber typedetector using the Li glass scintillator.
First of all, we evaluated the detector response at the E3
port of the Kyoto University Reactor. And then, the fab-

31P5-2

‑43‑

340
320
300
280
260
0.0
0.4
0.8
1.2
1.6
2.0
12 12
2
Thermalneutronfluence[×10
Integrated
thermalneutronfluence[x10n/cm
n/cm] 2]

Fig. 3. Time trend of the neutron peak channel during
irradiation with intense neutrons with the flux of
4x108 n/cm2/s.

35

1HXWURQPHDVXUHPHQWE\XVLQJWKHVHOIDFWLYDWLRQRILRGLQHDGGHGSODVWLFVFLQWLOODWRUVA. Nohtomi, Y. Hanada, G.Wakabayashi1, Y.Sakurai2 andT.Takata2*UDGXDWH6FKRRORI0HGLFLQH.\XVKX8QLYHUVLW\$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In our previous works, thermal
neutron was measured by using the self-activation of iodine-containing inorganic scintillators such as NaI andCsI [1, 2]. The method is highly sensitive even for shorttime irradiation, but not appropriate for very intense neutron field like the BNCT treatment, because the tuning ofsensitivity is not possible. Another drawback is the production of byproduct activity, 24Na and 134mCs. In thepresent work, the applicability of iodine-added plastic
scintillator was studied at rather intense neutron field like
BNCT one of KUR irradiation facility

Fig. 2. Pulse height distributions observed by the iodine-added plastic scintillators.
Figure 3 shows decay curves of count rate observed by
the iodine-added plastic scintillators. Only 128I decaying
components with half-life of 25 min are seen for both 1
wt% and 0.1 wt% scintillators. As clearly indicated in the
figure, no byproduct radio-activity is produced. This
property is very desirable for the application of iodine-added plastic scintillator to intense BNCT neutron
field.

(;3(5,0(176 Iodine-added plastic scintillator was
fabricated with an optical modeling type 3D printer(MiiCraft: MiiCraft Corp.). The base component was
M211-B and PPO; small amount of Bis-MSB and
Irgacure TPO are also mixed. In addition, iodobenzene(C6H5I) was added to the base material of plastic scintillator by 1 wt% and 0.1 wt% (Fig.1). Two plastic scintillators were irradiated at Rail Device of the Heavy Water
Neutron Irradiation Facility with OO-0000F mode
(1MW) [3]. Those scintillators were put at the Bismuth
Surface (thermal neutron flux : ~109 n/cm2/s) during 10
seconds for 1 wt% scintillator and 100 seconds for 0.1
wt% one. After the termination of each irradiation, theoutput signal of scintillators was read out by PMT and
MCA every one minute continuously.
5(68/76 Figure 2 shows pulse height distributions
observed by the two iodine-added plastic scintillators:1
wt% and 0.1 wt%. Reference spectrum of 128I beta-rays isalso indicated for comparison. Although iodobenzen is
known one of the strongest chemical quenchers, the shiftof pulse-height distribution towards low energy region is
not so significant because the amount added to plastic
scintillator is very small, but negligible.

Fig. 3. Decay curves of count rate observed by the iodine-added plastic scintillators.
$&.12:/('*(0(17 This work was supported
by JSPS KAKENHI Grant Number JP19K08202.
Dr. T. Kin and Mr. Y. Shinjyo of Kyushu University are
deeply appreciated for their fabrication of iodine-added
plastic scintillators.
5()(5(1&(6[1] G. Wakabsyashi HWDO, Radiol. Phys. Technol., (2015) 125-134.
[2] A. Nohtomi HWDO, JPS Conf. Proc.,  (2019)011041.
[3] Y. Sakurai and T. Kobayashi, Nucl. Instr. andMeth., $(2000) 569-596

Fig. 1. Appearance of iodine-added plastic scintillator.
(diameter : 25 mm, height : 25 mm)

31P5-4‑44‑

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Y. Sakurai1, N. Ko1,2, T. Takata1, H. Tanaka1, T. L. Tran3,
J. Davis3, S. Guatelli3, A. Rozenfeld3, N. Kondo1, M. Suzuki1

the p+ core and p+ ring detector when irradiated by themix irradiation mode of KUR-HWNIF are shown in Figs.
1 and 2, respectively. Higher events were observed withthe p+ ring detector, due to the larger surface area of thep+ region (i.e. absolute number of 10B atoms were larger).
The dominant component was the 1.47 MeV alpha particle, followed by the 840 keV 7Li ion. A small amount ofrecoil silicon was observed. The lineal energy was calculated and the yd(y) versus log(y) distribution was calculated, as shown in Fig. 3. From this spectrum, the p+ core
design had a higher lineal energy than the p+ ring and theprevious version microdosimeter (3D bridge).

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\.DQVDL%1&70HGLFDO&HQWHU2VDND0HGLFDO&ROOHJH&HQWUHIRU0HGLFDO5DGLDWLRQ3K\VLFV8QLYHUVLW\RI:ROORQJRQJ
,1752'8&7,21  Research and development into
several types of accelerator-based irradiation systems forboron neutron capture therapy (BNCT) is underway [1,2].
In the near future, BNCT using these newly developed
irradiation systems may be carried out at multiple facilities across the world. In contrast to conventional radiotherapy, the types of radiation present in BNCT consistsof many distinct radiation components, each having a
different biological weighting factor.
Microdosimetry is an effective dosimetry technique in amixed radiation environment. Using this technique, it ispossible to derive the relative contributions of different
radiation modalities. The feasibility study of a novel 3D
mesa bridge silicon-on-insulator microdosimeter (SIM) in
BNCT [3], developed by University of Wollongong(UOW).
In 2019, a new design silicon microdosimeter and its use
for dosimetry in boron neutron capture therapy (BNCT)
were investigatedby Monte Carlo simulation.

&21&/86,21 It was confirmed that the new detector can accurately measure the lineal energy of alpha particles emitted from the 10B(n,Į)7Li reaction.

Fig. 1. Deposit energy spectrum for the p+ core.

0(7+2'6 Two detector configurations were investigated, based on the current 3D mushroom microdosimeter. The first structure consists of a cylindrical p+ coreelectrode through the center of the SV with n+ ring electrode wrapped around the outside of the SV. The second
structure consists of a cylindrical n+ core electrodethrough the center of the SV with p+ ring electrodewrapped around the outside of the SV. Each SV has adiameter and height of 10 ȝm and the pitch between eachindividual SV is 40 ȝm to reduce cross talk between
neighboring row of detectors. A total of 2500 individual
SVs were connected in an array with odd and even detector row readout channels.
PHITS was used for this study. The T-deposit tally, whichscores dose and event-by-event deposition energy distribution was used to calculate the energy deposited inside
the SV of the mushroom microdosimeter. The microdosimetric spectrum (frequency mean and dose mean lineal
energy distribution) were calculated by dividing the deposited energy by the average chord length of the SV. The
detectors response to neutrons were investigated using
the neutron source for the mixed neutron irradiation of
Heavy Water Neutron Irradiation Facility installed in
Kyoto University Reactor (KUR-HWNIF).

Fig. 2. Deposit energy spectrum for the p+ ring.

Fig. 3. Microdosimetric yd(y) spectrum of the p+ coreand p+ ring detector, normalised to maximum.
5()(5(1&(6[1] H. Tanaka HW DO., Nucl. Instr. Meth. B  (2009)
1970-1977.
[2] H. Kumada HW DO., Appl. Radiat. Isot.  (2014)211-215.
[3] L. T. Tran HW DO., IEEE Trans. Nucl. Sci.  (2015)
3027-3033.

5(68/76 The deposit energy spectrum obtained with

31P5-6‑46‑

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35 7KH6WXG\IRU'HYHORSPHQWDQG$SSOLFDWLRQRI7LVVXH(TXLYDOHQW1HXWURQ'RVLPHWHU
M. Oita, T. Kamomae, T. TakaWaDQG <. Sakurai
*UDGXDWH 6FKRRO RI ,QWHUGLVFLSOLQDU\ 6FLHQFH DQG (QJLQHHULQJLQ+HDOWK6\VWHPV2ND\DPD8QLYHUVLW\*UDGXDWH 6FKRRO RI 0HGLFLQH 'HSDUWPHQW RI 5DGLRORJ\
1DJR\D8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Recent years, the clinical application of Accelerator-Based Boron Neutron Capture Therapy (AB-BNCT) has been introduced to make significant
contributions to treatment for intractable cancer such as
glioblastoma multiforme, superficial head and neck cancer, and melanoma in Japan.
In BNCT, the boron (n,α)-reaction of the isotope 10B has
a high cross-section toward thermal neutrons, and the
produced alpha and lithium particles have a short-range on
the micrometer scale. However, the neutron spec-trumalways spans a broad energy range, which results indifferent dose distribution and biological effects in tissue.
A radiochromic film (RCF) is one of the most useful dosimetry tools in the advantages of high spatial resolution,
small energy dependence, tissue equivalence, andself-development without processing in a darkroom1-3.
The hydrogel material is also expected to use for a patientbolus in clinical radiotherapy4. In this work, the authors
have developed new nanocomposite hydrogel for BNCT,
which is highly expected to use for a patient bolus inclinical BNCT.
Moreover, the hydrogel can improvedose distribution as well as can be manufactured arbitrary
size and thickness using a 3D printer.
Therefore, wehave investigated to develop a system that enables dose
optimization by optimally modulating the neutron beamfor each patient using the hydrogel and RCFs.
(;3(5,0(176Firstly, a reflective-type RCF,GAFCHROMIC® EBT3 (Ashland Inc., Wayne, NJ, USA)using a KUR neutron source was evaluated in this study.
For irradiation, 1.0 × 1.0 cm2 pieces of the RCF wereplaced at a depth of 0 cm to 24.2 cm in the air, wa-ter with
50ppm of boron, and water using the standard epithermal
neutron irradiation mode of the Heavy Water Neutron
Irradiation Facility at Kyoto University Research Reactor(KUR-HWNIF). Then, to assess the shielding effect of
the 3D printed hydrogel for neutron beam, test slabs were
fabricated.
The thickness and clay nanopar-ticles
concentration of the test slabs were varied from 2.5 to 5.2
wt%, respectively.
The irradiation experiment was
performed using KUR-HWNIF. Gold wires were used toestimate the neutron flux at the entrance and exit plane of
the test slabs. Thermo-luminescent dosimeters

31P5-9‑49‑

were used for the estimation of gamma-ray doses. The
measured data were normalized by the values at the entrance plane of the test slabs.
5(68/76  Fig.1 shows the change of relative pixel
values of RCFs irradiated by the KUR- HWNIF neutron
source. Further analysis was needed for the response of
RCFs with neutron components and contributions of
gamma rays using Monte Carlo simulation and additional
experiments with a cadmium filter.
Fig. 2 shows adepth neutron flux and gamma-ray distribution with achange in the clay nanoparticles concentration (left: 2.6
wt%, right: 5.2 wt%). The results showed that the influence of NC gel was mainly the neutron thermalization(Epithermal neutrons loss their kinetic energy). The
influence of the change in the clay nanoparticles concentration was almost unconfirmed.
These phenomena
would be affected by the buildup of neutron and gamma-ray doses. Our results demonstrated the feasibilityof utilizing the 3D printed compensator to modulate theneutron beam intensity for clinical BNCT.

Fig. 1 The change of relative pixel
values of the RCFs irradiated by
the KUR-HWNIF.

Fig. 2. Depth neutron flux and gamma-ray distribution withchange in the clay nanoparticles concentration. (left: 2.6 wt%,right: 5.2 wt%)

5()(5(1&(6>@ Niroomand-Rad, Azam HW DO. Medical physics
(1998), 2093-2115.
>@ Borca, Valeria Casanova HWDO. Journal of appliedclinical medical physics (2013).
>@ Fiandra, Christian HWDO Medical physics (2013).
>@ K Tanaka, Y Sakurai HW DO Applied RadiationandIsotopes (2017), 253-259.

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‑50‑

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-;8<<</-=387<"2//00/-=@+<+5<88,</;?/.37=2/8=2/;
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=2/$1/5.8<36/=/;< 
5()(5(1&(6>@ +5.8-4 /= +5 3K\V 0HG %LRO    E >@! +B+<23 /= +5 5DGLDW 0HDV    
106226>@  "+D8 /= +5 5DGLDW 0HDV LQ SUHVV    35 (VWDEOLVKPHQW RI EHDPTXDOLW\ HVWLPDWLRQ PHWKRG LQ %1&7 LUUDGLDWLRQ ILHOGXVLQJ GXDO SKDQWRPWHFKQLTXH ,,, 
Y. Sakurai, T. Takata, H. Tanaka, N. Kondo, M. Suzuki

5(68/76 Figures 2 and 3 show the depth distributions for the thermal neutron dose, fast neutron dose,
gamma-ray dose, and total dose in the LiF-polyethylene
phantom and the 6LiF-polyethylene phantom, respectively.
It was confirmed that the dose contribution of fast neutrons is improved from approximately 10% in the
LiF-polyethylene phantom, to approximately 50% in the6
LiF-polyethylene phantom.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Research and development into
several types of accelerator-based irradiation systems forboron neutron capture therapy (BNCT) is underway [1,2].
Many of these systems are nearing or have started clinical
trials. Before the start of treatment with BNCT, the relative biological effectiveness (RBE) for the fast neutrons(over 10 keV) incident to the irradiation field must be
estimated.
Measurements of RBE are typically performed by biological experiments with a phantom. Although the dose
deposition due to secondary gamma rays is dominant, therelative contributions of thermal neutrons and fast neutrons are virtually equivalent under typical irradiation
conditions in a water and/or acrylic phantom. Uniform
contributions to the dose deposited from thermal and fastneutrons is based in part on relatively inaccurate dose
information for fast neutrons.
The aim of this study is the establishment of accurate
beam-quality estimation method mainly for fast neutrons
by using two phantoms made of different materials, inwhich the dose components can be separated according todifferences in the interaction cross-sections. The fundamental study of a “dual phantom technique” for measuring the fast neutron component of dose is reported [3].
In 2019, verification experiments for the dual phantom
technique were performed using Heavy Water Neutron
Irradiation Facility installed in Kyoto University Reactor(KUR-HWNIF). Biological experiments were performed
using the solid phantoms, which were made based on thesimulation results in 2018.

&21&/86,21 The assay results are presently being
analyzed in association with the data of the depth dose
distribution for the thermal neutrons, fast neutrons andgamma-rays. The biological experiments using the othercell lines are under planning.
$&.12:/('*0(17 This work was supported by
JSPS KAKENHI Grant Number JP 16H05237.

Fig. 1. A schematic of the experimental setup.

0(7+2'6 One of the dual solid phantoms was madeof polyethylene with natural lithium fluoride for 30
weight percent (LiF-polyethylene phantom), and the other phantom was made of polyethylene with 95%-enrichedlithium-6
fluoridefor30
weightpercent(6LiF-polyethylene phantom).
Vials containing one kind of human brain cell, such as
U87ǻEGFR, were placed at the surface, 2-cm depth,
5-cm depth and 8-cm depth in the phantoms on the center
axis of the beam line. Cell growth assay was performed
for the irradiated cells.
The neutron flux and gamma-ray dose rate along the central axis in the phantoms were measured using activation
foils and thermo-luminescent dosimeter, respectively. The
depth dose distributions for the thermal neutron, fast neutron and gamma-ray components were determined basedon the simulation calculation results normalized referringto the measured values.
Figure 1 shows a schematic of the experimental setup.

Fig. 2. Depth dose distributions in the LiF-polyphantom.

Fig. 3. Depth dose distributions in the 6LiF-polyphantom.
5()(5(1&(6[1] H. Tanaka HW DO., Nucl. Instr. Meth. B  (2009)
1970-1977.
[2] H. Kumada HW DO., Appl. Radiat. Isot.  (2014)211-215.
[3] Y. Sakurai HWDO., Med. Phys.  (2015) 6651-6657.

31P5-11‑51‑

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35'HYHORSPHQWRI)LEHUUHDGLQJUDGLDWLRQPRQLWRULQJV\VWHPZLWKD
UHGLQIUDUHGHPLWWLQJVFLQWLOODWRUDW&RUDGLDWLRQIDFLOLWLHVS. Kurosawa1,2, S. Kodama2, T. Takada3, Y. Sakurai3, H.
Tanaka3

1HZ,QGXVWU\&UHDWLRQ+DWFKHU\&HQWHU7RKRNX8QLYHUVLW\,QVWLWXWHIRU0DWHULDOV5HVHDUFK7RKRNX8QLYHUVLW\ ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In the extremely high radiationdose condition such as inside of nuclear powerplant after
the accident (decommissioning), a real-time-remote radiation-monitor is required to survey the internal condition.
To avoid the radiation damage of the detectors or circuits,
the use of a long silica optical fiber (over ~100-m-length)
is proposed to read scintillation photons from the highdose condition [1] as shown in Fig. 1. To detect the scintillation photons efficiently through such a long opticalfiber, high-light output and red- or NIR-emitting scintillators are suitable than blue or yellow photons to suppress
the transmission loss.
We suggest to apply our developed red-emitting scintillator Cs2HfI6 (CHI) to the fiber-read radiation monitor
for the decommissioning. CHI has a broad scintillation
emission from 500 nm up to 800 nm with a peak ataround 700 nm, a short decay time of ~1.9 Ǎs among the
red-phosphors and high light output of 64,000 photons/MeV [2]. In this study, we demonstrated such fiber-reading systems under the high-dose condition at the60
Co Gamma-ray Irradiation Facility in Institute for Integrated Radiation and Nuclear Science, Kyoto University.

tillation photons.
The CHI and ruby-cement specimens were put on the
tip of an optical fiber (S.600/600B, Fujikura) with alength of 20 m and pure SiO2 core diameter of 600  30
Ǎm. The scintillation light was transmitted through thefiber and measured with a CCD spectrometer(Blue-UVNb, StellarNet). We determined the scintillation
signal intensity from the emission spectrum: integrationof the emission area. The exposure time of the CCD
camera was 5 sec for one time, and the measurements
were repeated three times for each dose rate position.
5(68/76 We succeeded in observation of emission
for CHI and also ruby with monitorable dynamic range of
10-2 up to 1 kSv/h for the first time, and emission intensities as a function of the dose rate are displayed in Fig. 2.
The data was linear-fitted by , = D[ + E, where , and [ arethe intensity and the dose rate, respectively, and coefficients (D, E) is (9.4x105, 3x103) and (1.4x105, 3x103) for
CHI and ruby, respectively.
The transition loss through the optical fiber for CHI
was larger than that of ruby due to slightly shorter emission peak; nevertheless, the scintillation signal of emission integrated area of CHI was the highest due to thehigh light output. Combining with the quick response
against gamma-rays with no afterglow, we should obtaina more accurate and reliable signal when CHI is used as a
scintillation prove than ruby. The detail of this collaboration study is described in [4].

Fig. 1 Schematic view of real-time dose monitor
Fig. 2Emission intensities for CHI and ruby excited by
gamma rays (60Co) as a function of the dose rate(;3(5,0(176 We prepared a small CHI piece witha size of 2 mm x 3 mm x 1 mm by Bridgeman method.
Due to hygroscopic nature, CHI was embedded in the
optical cement (BC-600, Saint-Gobain Crystal) with asize of 3 mm x 4 mm x 1.5 mm. The CHI-cement sample
was irradiated with gamma-rays from a 60Co source withan activity of ~100 TBq, and the gamma-ray air dose
rates at certain points on the experimental apparatus were
estimated by Sato et al.39). Also, we fabricated Cr-doped
D-Al2O3 sample (Ruby) with the same size and shapeincluding the cement as that of CHI to compare the scin-

5()(5(1&(6>@ C. Ito, et al., J. Nucl. Sci. Technol.  (2014) 944.
>@ S. Kodama, S. Kurosawa et al., Radiat. Meas. ,(2019) 54.
>@ N. Sato et al., (2008). at
http://www.rri.kyoto-u.ac.jp/gamma/doseratesheet.pdf>@ S. Kodama, S. Kurosawa and H. Tanaka et al., Applied Physics Express , (2020) 047002.

31P5-13‑53‑

35 Establishment of the Imaging Technology of 478 keV Prompt Gamma-rays of Boron-neutron
Capture Reaction and the Measurement of the Intensityof the Neutron Field
T. Mizumoto, S. Komura, Y. Sakurai1, A. Takada2,
T. Takata1, T. Tanimori2

urement results with E3 tube. Measurement was performed for two target positions. From the result, we cansee a clear positional difference between the two 478 keVgamma-ray images. We confirm 478 keV clear peak inspectra. Fig. 2 shows the schematic, photograph andmeasurement results with Heavy Water Neutron Irradiation Facility (epithermal neutron irradiation mode). The
gamma-ray flux is approximately 103 /cm2/sec in front of
the ETCC. Despite such the intense gamma-ray radiation
environment, where the conventional Compton cameras
are disturbed by random coincidence noise, our ETCC
succeeded to detect the 478 keV prompt gamma rays arrived from the water phantom target as we can see in the
spectra (a) and (b). In the prospects, we also need to try
the measurement test in the high neutron flux condition.

Fukushima SiC Applied Engineering Inc.
1
KURNS
2
Graduate School of Science, Kyoto University
INTRODUCTION:
BNCT is one of the promisingcancer treatment methods. However, we have not yet
obtained a good monitoring method of the treatment effect in real-time during BNCT. The main reason is that itis difficult to know precisely both the boron concentration and neutron flux intensity in tumor cells and healthy
ones. If we get images of 478 keV gamma-rays generated
by the boron-neutron capture reaction, and measure theirintensity and generation positions, we can check thetreatment effect on BNCT. To get gamma-ray images,
several detectors such as SPECT and Compton cameras
have been proposed. However, they have not been established due to their weaknesses [1]. To overcome the current situation, we have been developing electron tracking
Compton cameras (ETCCs) which can uniquely determine the arrival direction of sub-MeV/MeV gamma ray
event by event. An ETCC is the complex detector of two
sub detectors: a time projection chamber TPC (Compton
scatterer and recoil electron detector) and a scintillation
camera(scattering
gamma-rayabsorber)[2][3].
EXPERIMENTS: We developed an ETCC which has
a scintillation camera constructed with 576 pixelated
GSO scintillators, whose pixel size is 6 mm6 mm (26mm in high), and a TPC whose size is 330 cm2 (20 cm inhigh). As the performance measurement of the ETCC, we
carried out two types of measurements at the Institute forIntegrated Radiation and Nuclear Science, Kyoto University (KURNS). The first type was performed with E3
neutron guide tube of Kyoto University Reactor (KUR)(1 MW). We irradiated a Boron target (high concentration
Boron solution) with a thermal neutron beam from E3
tube. We set the ETCC near the target and measured
gamma rays from the target. The exposure time was a
few hours. Another type of measurement was performed
at KUR heavy water neutron irradiation facility. We set a(20 cm)3 Boron solution target in the irradiation room,and the ETCC on the ceiling of the room. We set both thetarget and the ETCC on the axis of the cylindrical holeabout 11 cm in diameter in the ceiling. We also set a LiFcontaining Teflon plate between the ETCC and the holeastheshieldingofthermalneutrons.
RESULTS: Fig. 1 shows the photograph and meas-

Fig.1. Photo and results of the experiment with E3
tube. Left: photo taken on the measurement. Right:
back-projection 478 keV gamma-ray images using the
ML-EM method and spectra taken by the ETCC.
Measurement was performed for two target positions.
The positional difference between A and B is 4 cm.

Fig.2. Schematic view, photograph and gamma-ray
energy spectra of the experiment with heavy water
neutron irradiation facility. ETCC measured gamma-rays from the treatment room. 10B concentrationof water phantom target is 250 ppm and 0 ppm.
REFERENCES:>@ 70L]XPRWR.85163URJUHVV5HSRUW  >@ <0L]XPXUD-,167  &
>@ 70L]XPRWR-,167  &

31P5-14‑54‑

35 )HDVLELOLW\ VWXG\ RI D JHOGRVLPHWHU IRU D TXDOLW\ DVVXUDQFH DQG D TXDOLW\ FRQWUROLQ ERURQQHXWURQFDSWXUHWKHUDS\S. Nakamura1,2, K. Iijima1, M. Takemori, H1. Nakayama1,
S. Nishioka1,2, H. Okamoto1,2, Y. Sakurai3, H. Tanaka3, N.
T. Takata3, M. Suzuki3, H. Igaki2,4, and J. Itami2,4
'HSDUWPHQWRI0HGLFDO3K\VLFV1DWLRQDO&DQFHU&HQWHU+RVSLWDO'LYLVLRQRI5HVHDUFKDQG'HYHORSPHQWIRU%RURQ1HX
WURQ&DSWXUH7KHUDS\1DWLRQDO&DQFHU&HQWHU([SORUDWRU\2QFRORJ\5HVHDUFK &OLQLFDO7ULDO&HQWHU,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\'HSDUWPHQWRI5DGLDWLRQ2QFRORJ\1DWLRQDO&DQFHU&HQWHU+RVSLWDO,1752'8&7,21  In boron neutron capture therapy(BNCT), the neutron irradiation to the patient is performed after a sufficient accumulation of 10B to tumor
cells because the treatment efficacy is based on the
10
B(n,α)7Li reaction. It is important for the radiation
therapy that the delivered dose is verified as a quality
assurance before the treatment. However, it is a difficult
for the existing detector that the three dimensional dose
distribution is measured in BNCT with considering a
non-uniformity of 10B on the actual patient. Thus, thisstudy focuses on the gel-dosimeter for the three dimensional dosimetry in BNCT. There are some reasons. First,
the gel-dosimeter can mix a few 10B with keeping thedose response. Second, the gel-dosimeter is generally
used for the three dimensional dosimeter. Third, thegel-dosimeter is not expensive, and the quality assurance
using the gel-dosimeter may not affect the medical costsin BNCT. Therefore, this study aims to evaluate the dose
response dependence of the gel-dosimeter which contains
a certain boron-10 density in BNCT.
(;3(5,0(176 The experiment was performed in
the Heavy Water Neutron Irradiation Facility (Kyoto
University Reactor, KUR). The KUR was operated at a
power of 1 MW. The neutrons were delivered to thegel-dosimeter which composed of water, PVA, KI, KCl,
Gellan gum, Fructose, and boron solutions. The boron-10
density of the gel-dosimeter was 0, 25, 50, and 75 ppm.
The irradiation time was set to 0, 5, 10, 15, 20, 30 min ineach gel-dosimeter. After the neutron irradiation, the dose
response in each gel-dosimeter was read by an opticalscanner. The dose response dependence in eachgel-dosimeter was evaluated.
5(68/76 Figure 1 (a) shows the dose responses ofgel-dosimeter in each boron-10 density and (b) shows
those in each irradiation time. According to Fig.1, thedose response increases with boron-10 density and irradiation time. Figure 2 shows the difference of dose response among the irradiation positions on the beam port.
The dose response of gel-dosimeter positioned at thecenter on the beam port was higher than that positioned at
the edge.
  'LVFXVVLRQ  This study suggests that thegel-dosimeter has a sufficient sensitivity for the reactionof 10B(n,α)7Li in BNCT although the boron-10 density
expects very low (25 ppm, etc«). According to fig. 1, thedose response in the gel-dosimeter increases with theboron-10 density and the irradiation time, and it seems
that the dose response can evaluate the actual dose delivered to the gel-dosimeter (Fig. 2). On the other hand, linearity of the dose response against the boron-10 density is
not sufficient. It may relate to a creating method of thegel-dosimeter. Some different method will be tried toseek the best method for creating the gel-dosimeter in the
future work.
&RQFOXVLRQ  We performed the feasibility test of thegel-dosimeter whether it could evaluate the three dimensional dose distribution in BNCT. The possibility for theevaluation could be indicated in this study. We will try tomeasure three dimensional dose in the future work.

(a) Dose response in each boron-10 density(b) Dose response in each irradiation time
Fig. 1 Dose response of gel dosimeterFig.2 Dependence of position

31P5-15‑55‑

35

2SWLPL]DWLRQRI%ROXV6KDSHIRU%RURQ1HXWURQ&DSWXUH7KHUDS\8VLQJ(SLWKHUPDO1HXWURQ%HDP

T. Takata, H. Tanaka, A. Sasaki1, Y. Sakurai, A.
Maruhashi and M. Suzuki

oral mucosa was fixed to be 12 Gy-Eq according to thetreatment protocol of BNCT for a head and neck cancer
performed at KUR. Under this condition, an objectivefunction was defined as the minimum dose of the PTV.
The bolus thicknesses were adjusted to maximize theobjective function by using a steepest gradient descentmethod.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\,1752'8&7,21  In Boron Neutron Capture Therapy (BNCT), epithermal neutron beam has been utilized totreat a deep-seated tumor due to its high penetration ability based on thermalization within a patient. However,thermal neutron buildup causes dose deficiency in a casefor a tumor locating in a vicinity of a patient surface. In
such a case, a bolus consisting of a hydrogen-rich material has been utilized to improve the dose distribution. In
present clinical BNCT, a bolus with a uniform thickness
and a simple shape has been adopted. Aiming to moreaggressively increase tumor dose, an optimizing methodof bolus shape was studied.

5(68/76 The location of the PTV and OAR isshown in Fig. 2. The control points were assigned to 43
surface voxels by using the method described above. The
iterative calculation was stared from bolus thicknesses ofzero at all control points. The result is shown in Fig. 3,
where increase and convergence in the PTV dose ac-cording to iteration are confirmed. Fig. 2 also shows
the resulting bolus shape at the 5th iteration, at which
the objective function is almost converged. The growthof the bolus was observed around the area under which
the PTV was extended into the subcutaneous region.

0$7(5,$/6 $1' 0(7+2'6 The optimization
was performed as following. At first, a beam incident
direction was determined according to location of a planning target volume (PTV) and organs at risk (OARs).
Then, control points to define bolus thicknesses wereassigned on the beam incident surface. A bolus region
was modeled in a patient geometry by interpolating the
thicknesses defined at the control points. These procedures were illustrated in Fig. 1. The thicknesses at thecontrol points were adjusted to maximize a PTV dose
under OAR dose regulations through an optimization
calculation. As an example, a case for parotid cancer extended into a subcutaneous region was examined.
3DWLHQW JHRPHWU\ PRGHOOLQJ: A PTV around a parotid
gland and an OAR for an oral mucosa were delineated on
X-ray CT images of a head phantom by a radiation oncologist. Then, a patient geometry model was constructed
for radiation transport calculations. A beam direction wasdetermined so that the PTV was centered in an irradiation
field while locating the OAR in a deeper side.
%ROXV IRUPDWLRQ: A bolus forming area was limited
within a surface area in a 5-cm distance from the beamincident point. Control points were assigned to voxels in
the area by using a 1.5 × 1.5 × 1.5 cm3 mesh-grid down
sampling method. A bolus region was generated in thepatient geometry by using an inverse-distance weighted
interpolation of the thicknesses of the control points.
1HXWURQ DQG SKRWRQ WUDQVSRUW FDOFXODWLRQ:
Thetransport calculations were performed by using a Monte
Carlo transport calculation module implemented in SERA; the treatment planning system for BNCT [1]. An
epithermal neutron beam of the KUR heavy water neutron irradiation facility with an aperture diameter of 12
cm was assumed in the calculations [2]. The results wereanalyzed by using a dose evaluation module of SERA.
2SWLPL]DWLRQ FDOFXODWLRQ: The maximum dose of theFig. 1. Procedure of bolus formation.

Fig. 2. Patient geometry with an optimized bobolus.

Fig.. 3. Change in the objective function accordi
according toan iterative calculation.
5()(5(1&(6>@ D. E. Wessol HWDO, INEEL/EXT-02-00698 (2002).
>@ Y. Sakurai, T. Kobayashi, Med. Phys.  (2002),
2328-2337

31P5-16‑56‑

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3

‑57‑

35 Measurement of neutron distributions in the BNCT irradiation field using a GEM detector
S. Uno, T. Koike, K. Miyamoto, K. Nobori, H. Tanaka

High Energy Accelerator Research Organization (KEK)  Faculty of Health Sciences, Kyorin University
 BeeBeans Technologies Co.Ltd
 Institute for Integrated Radiation and Nuclear Science,

Kyoto University
INTRODUCTION: The boron neutron capture therapy(BNCT) is a radiation therapy to destroy tumor cells selectively based on a nuclear reaction when 10B is irradiatedwith thermal neutrons. Epithermal neutrons are suitable
for the BNCT, because thermal neutrons are effectively irradiated on tumor cells after epithermal neutrons are moderated in the tissue. Therefore, it is important to know thespatial distribution of epithermal neutrons in the treatment
planning. For a measurement of the spatial distribution inthermal and epithermal neutrons irradiation field in the
BNCT, we have been developing a two-dimensional realtime imaging detector with the gas electron multiplier(GEM) [1]. The GEM is a position-sensitive device withthe gas amplification to detect charged particles, photons,
and neutrons. In this study, the performance of the GEM
detector was evaluated using the Heavy Water Neutron Irradiation Facility (HWNIF) of the Kyoto University Research Reactor (KUR) [2].
EXPERIMENTS: Our GEM detector has a compact bodywith dimensions, 444 mm × 270 mm × 41 mm. It consistsof a GEM chamber and a readout electronics board [3]. The
effective detection area is 100 mm × 100 mm. The ASIC
for the amplification and the FPGA for the online
processing are mounted on the electronics board, which isable to transfer data directly to a PC via the net-work. Fig.
1 shows a schematic cross-section of the GEM chamberwith a 10B-coated cathode plate. The detector works as agas radiation detector for neutrons by detecting thecharged particles emitted through a 10B(n, α)7Li nu-clear
reaction. Ionization electrons are created through theinteraction of the charged particle with the chamber gas in
the drift region and the electrons are amplified by the electron avalanche process which occurs at high electric fieldin GEM holes. The GEM is the double-side printed circuitboard, which consists of low temperature co-fired ceramic(LTCC) with 100 μm thickness as an insulator and gold
layers with 6 μm thickness on both sides as an electrode.
It has also a large number of holes with 100 μm diameterand 200 μm pitch (LTCC-GEM [4]). The LTCC-GEM isquite robust against the large discharge. Fig. 2 shows theexperimental setup of the GEM detector. In the clinicalpractice of the BNCT, a collimator with a diameter of 120
mm is normally used. In this study, the irradiation was
per-formed using an additional collimator with smalleraper-ture than the effective detection area to demonstrate
whether the detector can measure the neutron spatial distribution. In addition, the measurements were performed
while changing the detector position in order to observe theneutron flux distributions.

31P5-18‑58‑

Fig. 1. Cross-section of the GEM detector; electrons
are amplified in a succession of steps.

Fig. 2. Schematic diagram of experimental layout
and appearance of irradiation geometry at the HWNIF
of the KUR.
RESULTS: Fig. 3 shows the neutron spatial distribution
at a distance of 640 mm from the collimator surface andthe horizontal intensity profile at the beam center. The
beam condition of the neutron irradiation field could be
evaluated in real time and the collimator shape could beclearly seen. Since the detector is not sensitive against
gamma-ray, we guess that the tail of the distribution wascaused by neutron leaking from the collimator. For pulsed
neutron sources, the detector can measure the neutron energy distribution in the time-of-flight method, but for reactor neutron sources, the neutron generation time cannot
be determined because neutrons are randomly generated,so the neutron energy distribution cannot be measured. In
the future, we plan to make improvements so that the energy distribution of the reactor neutron sources can beevaluated.

Fig. 3. The neutron spatial distribution and the intensity profile at the beam center. The square blackline indicates the collimator size (60 mm × 50 mm).
REFERENCES:>@ F. Sauli, Nucl. Instrum. Meth. A 386 (1997)531.
>@ Y. Sakurai et al, Nucl. Instrum. Meth. A 453 (2000)569.
>@ S. Uno et al, Physics Procedia 26 (2012)142.
>@ K.Komiya et al, J. Jpn. Soc. Prec. Eng.84.11 (2018)936.

35

Development of Epi-thermal Neutron Flux Intensity Detector for BNCT

I. Murata, K. Aoki, Y. Miyaji, S. Kusaka, H. Tanaka1, Y.
Sakurai1 and T. Takada1
Graduate School of Engineering, Osaka University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: BNCT is a promising cancer therapy which kills tumor cells while suppressing exposure
dose to normal tissues. Normally, BNCT neutron field,
produced by a nuclear reactor or an accelerator-based neutron source, has energy distribution spreading within thermal, epi-thermal and fast neutron region. Because epi-thermal neutrons (0.5 eV<En<10 keV) are generally used for
BNCT, we must measure the epi-thermal neutron flux intensity to evaluate therapeutic effect and patients’ exposure dose. However, it is quite difficult to measure it directly and accurately because there is no available method
to measure the neutron spectrum and no activation materials covering only epi-thermal region. The objective of thiswork is hence to design a new detector to precisely measure the absolute integral flux intensity of epi-thermal neutrons.

Fig. 1.

Fig. 2.

Calculation model

Sensitivity of epi-thermal neutron detector

RESULTS: Measurement conditions are shown in Table.
1. The radioactivity immediately after irradiation of GaN
obtained by the experiment was 1.31 kBq. Therefore, theepi-thermal neutron flux intensity is estimated to be
1.76×108 n/cm2/sec by using Eq. (1). The nominal value of
epi-thermal neutron (0.5 eV<En<10 keV) flux intensity is
estimated to be 1.62×108 n/cm2/sec. Because this detector
is a little sensitive to fast neutrons, it is probable that a discrepancy seen between the experimental value and thenominal value.
To investigate the contribution from fast neutrons, we carried out a correction calculation by MCNP5. As a result,the amount of activation by fast neutrons was estimated to
be 50 Bq. Removing the contribution from fast neutron,
the radioactivity becomes 1.26 kBq. Then, the epi-thermal
neutron flux intensity is finally estimated to be 1.69×108
n/cm2/sec. It shows an excellent good agreement of 㹼4%.

EXPERIMENTS: The present epi-thermal neutron detector needs to reduce sensitivities to thermal and fast neutrons by using cadmium and polyethylene. We carried out
numerical simulations by MCNP5. As a result, 71Ga (n, γ)
72
Ga reaction was selected as the activation detector andthe shape of the epi-thermal neutron detector was fixed to
be a rectangular polyethylene (5.52 cm cubic) covered
with a cadmium sheet (Fig.1). The epi-thermal neutron detector is however a little sensitive to fast neutrons (Fig.2).
In order to test the performance of the epi-thermal neutron
detector, a verification experiment was conducted at KUR.
After the experiment, we can know the epi-thermal neutron flux intensity by Eq. (1). All we have to do is to measure radioactivity of 72Ga, meaning it is easy and it takes ashort time.

Table. 1.

Measurement conditions.

CONCLUSION: The epi-thermal neutron flux intensity
could be measured with an error of 4.2 % by correctingwith the calculated value in the experiment at KUR. In order not to carry out a correction, we are developing a fastneutron (10 keV<En<1 MeV) flux intensity detector.

31P5-20‑59‑

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$QDO\]LQJ7XPRU0LFURHQYLURQPHQWDQG([SORLWLQJLWV&KDUDFWHULVWLFVLQ
6HDUFKRI2SWLPL]LQJ&DQFHU7KHUDS\,QFOXGLQJ1HXWURQ&DSWXUH7KHUDS\

Shin-ichiro Masunaga,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\%$&.*5281'6$1'385326(6Human solid tumors contain moderately large fractions of quiescent (Q)tumor cells that are out of the cell cycle and stop cell division, but are viable compared with establishedexperi-mental animal tumor cell lines. The presence of Q
cells is probably due, in part, to hypoxia and thedepletion of nu-trition in the tumor core, which is anotherconsequence of poor vascular supply. As a result, Q
cells are viable and clonogenic, but stop cell division. In
general,radiationandmany
DNA-damaging
chemotherapeutic agents kill prolif-erating (P) tumor cells
more efficiently than Q tumor cells, resulting in manyclonogenic Q cells remaining following radiotherapy or
chemotherapy. Therefore, it is harder to control Q
tumor cells than to control P tumor cells, and many
post-radiotherapy recurrent tumors result partly fromthe regrowth of Q tumor cells that could not be killed byradiotherapy. Similarly, sufficient doses of drugs cannot
be distributed into Q tumor cells mainly due to heterogeneous and poor vascularity within solid tumors. Thus,
one of the major causes of post-chemotherapy recurrent
tumors is an insufficient dose distribution into the Q cell
fractions.
With regard to boron neutron capture therapy (BNCT),
with B-compounds, boronophenylalanine-B (BPA) increased the sensitivity of the total cells to a greater
extent thanmercaptoundecahydrododecaborate-B(BSH). However, the sensitivity of Q cells treated with
BPA was lower than that in BSH-treated Q cells. The
difference in the sensitivity between the total and Q
cells was greater with B-compounds, especially with
BPA. These findings concerning the difference insensitivity, including other re-covery and reoxygenation
following neutron irradiation after B-compound
administration were mainly based on the fact that it isdifficult to deliver a therapeutic amount of B from Bcarriers throughout the target tumors, es-pecially into
intratumor hypoxic cells with low uptake ca-pacities.
Hypoxia is suggested to enhance metastasis byincreas-ing genetic instability. Acute, but not chronic,
hypoxia was reported to increase the number ofmacroscopic metastases in mouse lungs. We recently
reported the significance of the injection of an acutehypoxia-releasing agent, nicotin-amide, into tumorbearing mice as a combined treatment with J-ray
irradiation in terms of repressing lung metasta-sis. As thedelivered total dose increased with irradiation, thenumber of macroscopic lung metastases decreased reflecting the decrease in the number of clonogenically viable tumor cells in the primary tumor. The metastasis-repressing effect achieved through a reduction in thenumber of clonogenic tumor cells by irradiation is muchgreater than that achieved by releasing tumor cells fromacute hy-poxia. On the other hand, more B from BPA
than from BSH could be distributed into the acutehypoxia-rich total tumor cell population, resulting in agreater decrease in the number of highly clonogenic P
tumor cells with BPA-BNCT than with BSH-BNCT andwith neutron beam irra-diation only. BPA-BNCT rather
than BSH-BNCT has some potential to decrease thenumber of lung metastases, and an acute hypoxiareleasing treatment such as the ad-ministration of
nicotinamide, bevacizumab, wortmanninor thalidomide may be promising for reducing numbers oflung metastases. Consequently, BPA-BNCT in combination with the treatment using these agents may show a little
more potential to reduce the number of metastases. Now,
it has been elidated that control of the chronic hypoxiarich Q cell population in the primary solid tumor has thepotential to impact the control of local tumors as a whole,and that control of the acute hypoxia-rich total tumor cell
population in the primary solid tumor has the potential toimpact the control of lung metastases.
The aim of this research project is focused on clarifying and analyzing the characteristics of intratumor microenvironment including hypoxia within malignant solid tumors and optimizing cancer therapeutic modalities, especially radiotherapy including BNCT in the use of newlydeveloped B-carriers based on the revealed findings on
intratumor microenvironmental characteristics.
5(6($5&+68%-(&76
The collaborators and allotted research subjects (ARS)
were organized as follows;$56 3 : Optimization of Radiation Therapy Including BNCT in terms of the Effect on a Specific Cell
Fraction within a Solid Tumor and the Suppressing Effectof Distant Metastasis. (S. Masunaga,HWDO)$56 3 : Development of Hypoxic Microenvironment-Oriented B-Carriers. (H. Nagasawa, HWDO)$56 3 *: Search and Functional Analysis ofNovel Genes that Activate HIF-1, and Development into
Local Tumor Control. (H. Harada, HWDO)$56 3 : Radiochemical Analysis of Cell Lethality Mechanism in Neutron Capture Reaction. (R.
Hirayama, HWDO)$56 3 : Development of Neutron Capture Therapy Using Cell-Membrane Fluidity Recognition Type
Novel Boron Hybrid Liposome. (S. Kasaoka, HWDO)$56 3 : Drug Delivery System Aimed at Adaptation to Neutron Capture Therapy for Melanoma. (T.
Nagasaki, HWDO)$56 3 : Molecular Design, Synthesis and Functional Evaluation of Hypoxic Cytotoxin Including Boron.
(Y. Uto, HWDO)$56 3 : Bystander Effect on Malignant Trait ofTumor Cells by Irradiation. (H. Yasui, HWDO)$56 3 : Analysis of the Response of Malignant
Tumor to BNCT. (M. Masutani, HWDO)$56 3 : Cell Survival Test by Neutron Capture
Reaction Using Boron Compound and Inhibitory Effecton Tumor Growth. (K. Nakai, HWDO)$56 3 : Multilateral Approach Toward
Realization of Next Generation Boron Neutron Capture
Therapy. (Y. Matsumoto, HWDO)$56 3 : Analysis of Radiosensitization Effectthrough Targeting Intratumoral Environmental. (Y.
Sanada, HWDO)$56 3 *: Exploratory Research on the Optimal Administration of 10B Compound Aiming at New Enforcement Method of Neutron Capture Therapy (S.
Masunaga HWDO.)$56 3 *: Examination of Cancer Cell Accumulation Property of New Boron Agent (CbaP14). (J.
Hiratsuka,HWDO)(*There was no allocated time for experiments using reactor
facilities during their operation periods of FY 2019.

3
‑62‑

35

(IIHFWRIDFKDQJHLQUHDFWRUSRZHURQUHVSRQVHRIPXULQHVROLGWXPRUVin vivo
HVSHFLDOO\RQWKDWRITXLHVFHQWWXPRUFHOOVLQERURQQHXWURQFDSWXUHWKHUDS\power of 1MW and in total cells, respectively. The sensitivity difference between total and Q cells was widened when combined with 10B-carrier, especially with
BPA, and through decreasing reactor power.

S. Masunaga, Y. Sakurai, H. Tanaka, T. Takata, M.
Suzuki, Y. Sanada, K. Tano, A. Maruhashi and K.Ono
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\.DQVDL%1&70HGLFDO&HQWHU2VDND0HGLFDO&ROOHJH

&21&/86,21: In actual clinical situations, it takes
approximately 5 times longer time at a power of 1MW
than 5MW to carry out one session of BNCT. Patients,1752'8&7,21 Neutron beams, that are essential cannot move their body at the optimum treatment posifor performing BNCT, have been supplied at some re- tion all through the treatment time for BNCT. Thus, it issearch reactors. In Japan, based on legal regulations, very reasonable that reactor power was maintained atmore reactor operation personnel have to be in place at 5MW for BNCT even after the power during reactor opthe time of high power reactor operation (5 MW), than eration for research use was reduced to 1 MW. Consewith low output operation (1 MW). In our reactor, to quently, taking these findings obtained in the current LQprevent nuclear fuel from being depleted during the re- YLYR studies and clinical realities into consideration,
actor operable period, the output power during reactor 5MW is more useful, convenient, appropriate, advantaoperation for research use has been reduced from 5 to geous and practical than 1MW as a reactor operation
1MW since 2010. However, reactor operation output re- power in clinical BNCT [4].
mains at 5MW at the time of clinical boron neutron capture therapy (BNCT) to prevent prolongation of irradiation time.
We analyzed the changes in the values of relative
biological effectiveness (RBE) for neutron-only irradiation and compound biological effectiveness (CBE)factors for employed 10B-carriers according to the value ofa power of the operated reactor [1,2]. The neutron
capture reaction was performed with two kinds of 10B(BPA,
carriers,boronophenylalanine-10B
10
C9H12 BNO4) or sodium mercaptoundecahydrodo(sodium
borocaptate-10B,
BSH,
decaborate-10B
Na210B12H11SH). Regarding local tumor response, theeffect not only on the total [proliferating (P) + quiescent(Q)] tumor cell population, but also on the Q cell population, was evaluated using our original method for selectively detecting the response of Q cells in solid tumors [3].
0$7(5,$/6 $1' 0(7+2'6 SCC VII tumorbearing mice continuously received 5-bromo-2’-deoxyuridine (BrdU) to label all P tumor cells, and weretreated with BPA or BSH. After reactor neutron beamirradiation at a power of 1 or 5MW with an identicalbeam spectrum, cells from tumors were isolated and incubated with a cytokinesis blocker. The responses of
BrdU-unlabeled Q and total (P + Q) tumor cells were 5()(5(1&(6>@ R F. Barth HWDO5DGLDW2QFRO (2012) 146–
assessed based on the frequencies of micronucleation
166.
using immunofluorescence staining for BrdU.
>@ JW. Hopewell HWDO in 1HXWURQFDSWXUHWKHUDS\3ULQFLSOHVDQGDSSOLFDWLRQV Edited by W. Sauer5(68/76 After neutron irradiation with or without
wein, A. Wittig, R. Moss, Y. Nakagawa (Springer10B-carrier, radio-sensitivity was reduced by decreasing
Verlag, Berlin, 2012) pp. 329–358.
reactor power in both cells, especially in Q cells and af-ter>@ S. Masunaga and K. Ono -5DGLDW5HV
irradiation with BPA. The values of RBE and CBE were(2002)11–25.
larger at a power of 5MW and in Q cells than at a
>@ S. Masunaga HWDO ,QW-5DGLDW%LRO (2019)645.

31P6-1‑63‑

35'HYHORSPHQWRIQHZDPLQRDFLGW\SHERURQFDUULHUVIRU%1&7

A. Matsushita, M. Tsuji, Y. Sanada, T. Hirayama,
S. Masunaga and H. Nagasawa/DERUDWRU\RI0HGLFLQDO 3KDUPDFHXWLFDO&KHPLVWU\*LIX3KDUPDFHXWLFDO8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In malignant tumor cells, there isa significant increase in the demand for amino acids tomaintain rapid growth and energy metabolism, and inparticular such cancer cells show glutamine addiction.

found that compound  (41 ng 10B/106 cells) and (206ng 10B/106 cells) showed significantly higher uptake than
BPA (23 ng 10B/106 cells).
To evaluate neutron sensitizing ability of the compounds,
T98G cells were treated with 10 μg 10 B/mL boron carriers for 24 h. Then the cells were washed with PBS, suspended in serum containing medium and aliquoted into
Teflon tubes for irradiation. Cells were irradiated using
the neutron beam at the Heavy Water Facility of the
Kyoto University Research Reactor (KUR) operated at 1
MW power output. The survival rates of the irradiatedcells were determined using conventional colony assays.
The D10 of BNCT was calculated from survival curve
shown in Fig. 2.
Radiation dose (Gy)
0

1

2

3

Survival fraction

1

Fig. 1. Metabolic shift in malignant tumor cellsThus, such tumor cells overexpress transporters (ASCT2and LAT1) that transport glutamine and neutral aminoacids with aromatic or branched side chains. In this study,
we designed and synthesized boron cluster-containing
amino acid derivatives for the purpose of developing boron carriers that can efficiently capture 10B atoms in tumors using tumor-specific amino acid transporters, focusing on glutamine addiction in cancer.

0.1
controlBPA
1
2

control

0.01

BPA
1
2
0.001

(;3(5,0(176 $1' 5(68/76 First, utilizing boron clusters as unique hydrophobic pharmacophores, we
synthesized carborane(C2B10H12)-containing amino acid
L-R-carboranylalanine()andderivatives
2-(R-carboran-1-ylmethyl) -L-tyrosine (), which mimic
the transport substrate of LAT1. They were efficiently
obtained from the corresponding amino acid alkynes anddecaboran in a short step using our microwave-assisted
reaction, with total yields of 53% and 46%, respectively.
Rm values of all compounds were examined by TLC
method (RP-8 modified silica gel TLC, 20 mM phosphatebuffer (pH 7.2) : methanol = 7:3) as hydrophobic parameter.

Next, the uptake of boron atoms was evaluated after
treatment of T98G with these compounds andL-boronophenylalanine(BPA). Intracellular boron uptake
was measured by ICP-AES after 20 h of treatment with
10 μg 10 B/mL of the boron carriers. As a result, it was

31P6-2‑64‑

Fig. 2. Survival fraction of T98G cells treated with compound ,  and BPA and irradiated by mixed-neutron
bean for BNCT.
Table 1. Intracellular uptake of 10B atom, Rm values, D10values and the enhancement ratios of boron carriers.
10

Compoundcontrol
BPA
1
2

B uptake( B ng/106 cells)
nd
23
41
203
10

Rm value
䞊
nd
0.302
1.09

D10 value enhancement
ratio
(Gy)
6.41
1.00
3.31
1.94
2.85
2.25
0.25
25.8

In summary, Compound  showed approximately
9-fold higher intracellular 10B uptake than BPA. In addition,compound  enhanced the inhibition of cell survivalof T98G cells irradiated with thermal neutrons by 13-foldcompared to BPA. These results suggest that  is a promising candidate for new boron carrier. We are now synthesizing more diverse derivatives and investigating thestructure-activity relationship analysis in BNCT.

35

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35

2+UDGLFDOVIURPWKHLQGLUHFWDFWLRQVRIQHXWURQEHDP LQGXFHFHOONLOOLQJ
ing DMSO concentration and then plateaued at higher
concentrations (Fig.1A). Degrees of protection (DP:(lnSF0-lnSFx)/lnSF0) defined was calculated and plotted
as a function of the DMSO concentration (Fig. 1B). Since
the curve were upper concave in nature, DP curve wasapproached saturation as the concentration of DMSO
increased. The maximum DP (i.e., saturation level) for
DMSO concentrations was 0.29. Namely, the OH radical-mediated indirect action contributions to cell killingby neutron beam was 29%.

R. Hirayama, Y. Sanada1, A. Uzawa, M. Suzuki1, S.
Masunaga1 and S. Hasegawa
1DWLRQDO,QVWLWXWHRI5DGLRORJLFDO6FLHQFHV 1,56 1D
WLRQDO,QVWLWXWHVIRU4XDQWXPDQG5DGLRORJLFDO6FLHQFH
DQG7HFKQRORJ\ 467
 ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ .8516,1752'8&7,21 Excellent dose distribution in acell of neutron capture reaction of boron atom induceshigh relative biological effectiveness. These phenomena
are commonly assumed to be an interaction between cells
and low energy KHDY\SDUWLFOHV ĮDQG/L UHVXOWLQJIURPthe boron atom fis-sions in the cells. However, there has
been little study done concerning the action of the particles on living cells. We have investigated contributions of
indirect actions of radiation in cell killing by heavy ionswith radical scavenger that selectively reduces the indirect action [1].
Therefore, it is important that how these mechanisms
can be made to clear through a thorough basic research inboron neutron capture therapy is urgently discussed. The
main object of this year is to make clear the contributionof indirect action of neutron beam to cell killing using
mammalian cells.
(;3(5,0(176 We used HSGc-C5 (JCRB1070,here
after call as HSG) cells. HSG cells were grown in Eagle’s
minimum essential medium supplemented with 10% fetal
bovine serum and antibiotics (100 U/ml penicillin and100 μg/ml streptomycin) under humidified air with 5%
CO2 DW Û&. The cells were suspended at a density of
about 3 × 105 cells/ml. The cells in Polypropylene tubes
were irradiated at the remodeled heavy water facility at
the KURRI.
Total fluencies of thermal neutron, epithermal neutronand fast neutron were measured by means of gold foil
activation analysis. The gamma ray dose including secondary gamma rays was measured with a thermo luminescence dosimeter. Boron concentrations in the cells
were taken to be equivalent to those in the medium asreported previously [2].
After irradiation, cells were seeded in triplicate onto
10 PP ĭ  FXOWXUH GLVKHV DW GHQVLWLHV WR JLYH DSSUR[L
mately 100 colonies per dish. After 14 days of incubation,
the colonies were fixed with 10 % formalin solution andstained with 1 % methylene blue in water. Colonies consisting of more than 50 surviving cells were scored.
The contribution of indirect action on cell killing canbe estimated from the maximum degree of protection bydimethylsulfoxide (DMSO) [1], which suppresses indirect action by quenching OH radicals without affecting
the direct action of neutron beam on cell killing.

A

B

Fig. 1. Effects of DMSO on the survival of HSG
cells after exposure to neutron beam. (A) HSG cell
survival irradiated with neutron beam in the presenceof various concentration of DMSO. (B) Degrees ofprotections were determined from panel A. The
curve was fitted by MichaelisMenten kinetics. The
error bars represent the standard errors.
5()(5(1&(6[1] R. Hirayama HWDO, Radiat. Res., (2009) 212-218.
[2] Y. Sakurai and T. kobayashi, Nucl. Instrum. Methods
Phys. Res. Sect. A., (2000) 569-596.

5(68/76 The surviving fractions of HSG cells irradiated with 5.85 Gy dose initially increased with increas-

31P6-4‑66‑

35,QWUDFHOOXODU'HOLYHU\RI0HPEUDQHIOXLGLW\6HQVLWLYH%RURQ/LS
RVRPHVZLWK7XPRUVSHFLILF&HOO3HQHWUDWLQJ3HSWLGHVS. Kasaoka, M. Saruwatari, Y. Tanaka, Y. Sanada, Y.
Sakurai, H. Tanaka and S. Masunaga
'HSDUWPHQWRI3KDUPDFHXWLFDO6FLHQFH+LURVKLPD,Q
WHUQDWLRQDO8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
There are many reports that
membranes in cancer cells are relatively more fluid compared to healthy cells. Higher membrane fluidity in cancer cells closely relates to their invasive potential, proliferation, and metastatic ability [1]. Liposomes composedof dimyristoylphosphatidylcholine (DMPC) and polyoxyethylenedodecylether were found to inhibit the growthof human promyelocytic leukemia cells without using
any drugs [2]. Cell-penetrating peptides (CPPs) havebeen studied for their capacity to translocate across thelipid membrane of several cell types. 17-amino acid cell
penetrating peptide (BR2) was found to have cancer-specificity without toxicity to normal cells [3]. In thisstudy, we have developed a novel boron delivery systemusing the membrane-fluidity sensitive boron liposomes(MFSBLs) composed of DMPC and borocaptate(BSH)-conjugated chemical compounds with cell penetrating peptides (BR2) for boron neutron capture therapy.
(;3(5,0(176
2FWDGHF\ODPLQH
DQG

GLP\ULVWR\OVQJO\FHURSKRVSKRU\OHWKDQRODPLQH
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FRQMXJDWHG 0)6%/V FRPSRVHG RI '03&
SRO\R[\HWK\OHQHGRGHF\OHWKHU ERURQ FRPSRXQGV DQG%5 DW PROH UDWLRV RI  ZHUH SUHSDUHG E\
VRQLFDWLRQ PHWKRG LQ  JOXFRVH VROXWLRQ  DW &
7KH GLDPHWHU RI 0)6%/ V ZDV PHDVXUHG ZLWK D OLJKWVFDWWHULQJ VSHFWURPHWHU 7KH ERURQ FRQFHQWUDWLRQ ZDVPHDVXUHGE\LQGXFWLYHO\FRXSOHGSODVPDDWRPLFHPLVVLRQVSHFWURPHWU\ %) PXULQH PHODQRPD FHOOV DQGKXPDQ ILEUREODVW FHOOV ZHUH LQFXEDWHG ZLWK  SSP RI
 % DW & IRU  KRXUV EHIRUH QHXWURQ LUUDGLDWLRQ
7KH FHOOV ZHUH ULQVHG WZLFH LQ 3%6 DQG VXVSHQGHG LQ
IUHVK PHGLXP$IWHU QHXWURQ LUUDGLDWLRQ WKH FHOOV ZHUH
SODWHG LQWR SODVWLF 3HWUL GLVKHV  PP LQ GLDPHWHU DW FHOOV SHU GLVK 7KH\ ZHUH LQFXEDWHG IRU DQ DGGLWLRQDOGD\VWRDOORZFRORQ\IRUPDWLRQ

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‑67‑

5(68/76 Tumor-specific CPPs (%5  FRQMXJDWHG
MFSBLs had a mean diameter of 78.5 nm. High encapsulation efficiency value from 48% to 74% of 10B in
MFSBLs were obtained. %5VFRQMXJDWHGMFSBLs hadhigh stability (92-97%) in the retention of 10B duringstorage at 4°& for 4 weeks. All borocaptate-loaded formulations had low cytotoxic effects in human fibroblast
cells. %5FRQMXJDWHG were efficiently fused to melanoma cells, but were inefficiently fused to human fibroblast cells. As shown in Fig. 1, BR2-conjugated MFSBLs
showed higher suppression of growth of murine and human melanoma cells than BSH solution. This result suggested novel BR2-conjugated MFSBLs is useful for 10B
carrier on BNCT for melanoma.

Fig. 1. Suppression of the colony formation of B16F10
cells and fibroblast cells after in vitro BNCT.
5()(5(1&(6>@ Sherbet GV. Magalit, Exp Cell Biol. (1989)
>@ Y. Matsumoto et al. Int. J. Cancer,  (2005)
>@ K. Lim et al. PLoS One,  (2013)

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35

Development of novel BPA-Tirapazamine hybrid BNCT
agent targeting hypoxic tumor cells

Y. Uto, Y. Tanaka, S.Masunaga1, Y.Sanada1
Graduate School of Technology, Industrial and Social
Sciences, Tokushima University
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.XR\R8QLYHUVLW\INTRODUCTION:
Hypoxia is a ubiquitous environment of cancer, it has aresistance to anticancer drugs and X ray, and accelerated
infiltration / metastasis is a problem. Boron neutron capture therapy (BNCT), a kind of radiotherapy, is a treatment method utilizing neutron capture reaction in tumor
cells by accumulating 10B in tumor tissue. Hybrid molecules of Tirapazamine (TPZ), as a hypoxic cytotoxin andthe neutron scavenger p-borono-L-phenylalanine (BPA)
are useful as selective neutron scavengers for hypoxic
tumors. Since boron neutron capture therapy depends on

Fig.2
Toxicity test was performed by WST-1 assay using
HeLa cells. As shown in Table 1, UTX-118 exhibitedhypoxia-selective toxicity. The low toxicity of UTX-117
may be due to low uptake.
Normoxia
Hypoxia
UTX-117>1000 μM
299 μM
UTX-118
24.4 μM
7.17 μM
TPZ
346 μM
21.1 μM
N/H ratio=the IC50 value of Normoxia/ the IC50 value of Hypoxia

10

B concentration, it is expected to provide an effective
therapeutic effect for hypoxic cancer.
In this study, UTX-117 with amide linkage of TPZ and
BPA and UTX-118 with ester linkage of TPZ and BPA
were designed and synthesized, and antitumor activity
and neutron sensitizing activity were evaluated. UTX-118
exhibited
hypoxiaselective
cytotoxicity.
Further, UTX-118 showed neutron sensitizing activity.

Table. 1

EXPERIMENTS:
Tirapazamine derivatives and BPA were condensed tosynthesize UTX-117 and UTX-118 (Fig.1). Using HeLa
cells, the uptake amount of UTX-117 and UTX-118 was
measured by ICP-AES, and the intracellular boron concentration was calculated. The IC50 values of UTX-117
and UTX-118 were calculated by WST-1 assay. Afteradding 10B enriched UTX-117, 10B enriched UTX-118
and 10B enriched BPA-F (>99.5% 10B) to HeLa cells,
neutrons were irradiated to calculate cell viability.

UTX-117

N/H ratio
3.40
16.4

Neutron sensitizing activity of 10B enriched UTX-117,
B enriched UTX-118 and 10B enriched BPA-F was
evaluated using HeLa cells (Fig. 3). 10B enriched
UTX-118 showed the neutron sensitizing activity (sensitization ratio: 4.15 compared to the neutron irradiation
control group). Since the sensitization ratio of 10B enriched BPA-F was 3.27, 10B enriched UTX-118 showed
higher neutron sensitization activity than 10B enriched
BPA-F.
10

UTX-118
Fig.1

RESULTS:The uptake test of UTX-117, UTX-118 and BPA-F was
performed using HeLa cells (Fig. 2). The boron concentration required for BNCT is 1.0 × 109 atoms / cell.[1]since the maximum uptake of UTX-118 was approximately 1.0 × 109 atoms / cell, a neutron sensitization effect can be expected for UTX-118. On the other hand,
UTX-117 was below the detection limit of ICP-AES.

Fig.3. +:Irradiation, -:Non-irradiation
REFERENCES:>@ F. F. Flores et al. Radiat. Environ. Biophys.  201232931P6-7‑69‑

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H. Yasui, M. Eitaki, S. Masunaga and O. Inanami

Green Master (Roche) according to the manufacture’s
instruction. GAPDH was used as an internal control.
Amount of mRNA was expressed as relative values
which set that of non-treated cells to 1.

/DERUDWRU\RI5DGLDWLRQ%LRORJ\*UDGXDWH6FKRRORI
9HWHULQDU\0HGLFLQH+RNNDLGR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In cancer studies, it has been suggested that irradiation sometimes enhances invasion oftumor cells. Wild-Bode et al. reported that sublethal doseof Ȗ-ray irradiation enhanced invasiveness of human glioblastoma, and the enhancement was accompanied by theactivation and/or up-regulation of integrin and matrix
metalloproteinase (MMP) contributed to cellular adhe-sionand degradation of extracellular matrix (ECM) [1]. Fujita
et al. also reported that X-ray irradiation enhanced cellularinvasive ability via up-regulation of MMP in some humanpancreatic tumors [2]. Including these re-ports, a numberof studies suggested that ECM degrada-tion activity was
involved in the irradiation-enhanced invasiveness of tumor
cells. However. although there are many studies that
estimate effects of direct irradiation on tumor cell
invasiveness, not so many reports did by-stander effects ofirradiated tumor cell conditioned me-dium (CM) on it.
Furthermore. the same effect of high LET radiation therapy such as boron neutron capture reaction (BNCT) has
not been reported. In this study, we conducted the experiments to examine effects of X-irradiated tumor cellCM on cellular invasiveness in breast cancer and lungcancer-derived cells, prior to BNCT challenge. In 2018,using human breast adenocarcinoma MDA-MB-231 cells
and human lung adenocarcinoma A549 cells, we reported
the X-ray irradiated ce1l-derived CM promotes cell infiltration ability even if taken into consideration cell proliferation activity [3]. In this year, we examined the expressions of growth factors such as Epidermal growth factor(EGF), Vascular endothelial growth factor (VEGF) andTransforming Growth Factor-ȕ1 (TGF-ȕ1) in X-irradiated
MDA-MB-231 cells.
(;3(5,0(176 The expression of growth factors
was evaluated using real-time PCR. Cells were seeded on
60 mm dishes (1 × 106 cells/dish), and incubated with
RPMI1640/10% FBS overnight. After washing by PBS, 2
ml of serum-free RPMI1640 medium was added to thedishes followed by 0 or 4 Gy X-irradiation immediately.
After 0-24 h incubation, the cells were collected withtime. Total RNA of the cells was extracted by SV Total
RNA Isolation System (Promega, Madison, WI.) according to the manufacture’s instruction. RNA concentration
was measured by DU 800 (BECKMAN COULTER, CA.).
Reverse transcription was performed by Reverse Transcription System (Promega) according to the manufacture’s instruction. Real-time PCR was performed byLightCycler® Nano System (Roche Diagnostics GmbH,
Mannheim, Germany) and FastStart Essential DNA

P6-8‑70‑

5(68/76 Since the CM derived from X-ray-irradiatedcells promoted the cell invasion ability [3], it was considered that some bystander factor that promotes thecell-infiltrated ability exists in the CM derived fromX-irradiated cells. Therefore, using MDA-MB-231 cells,
which showed a large effect of promoting invasion ability
by CM derived from X-ray-irradiated cells, the expression of mRNA for several proteins related to invasion
ability in non-irradiated and 4 Gy-irradiated cells wasmeasured using real-time PCR method. As shown in Fig.
1., the mRNA levels of TGF-ȕ and VEGF were not increased by at least 24 hours in 4 Gy-irradiated cells compared to non-irradiated cells. On the other hand, theamount of EGF mRNA was significantly increased in the
4 Gy-irradiated cells with a peak at 18 hours after
X-irradiation. This result suggested that EGF acts as a
bystander factor to promote the cell invasion ability.

Fig. 1. The time-course of the mRNA expression of
EGF, VEGF, and TGF-ȕ in X-irradiated
MDA-MB231 cells. *; p < 0.05 YV non-irradiatedcells
5()(5(1&(6[1] C. Wild-Bode HWDO, Cancer Res., (2001) 2744-50.
[2] M. Fujita HWDO, Cancer Sci., (2011) 729-8.
[3] H. Yasui HWDO, KURNS Progress Report 2018, PR8-7.

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Y. Sanada, T. Takata, Y. Sakurai, H. Tanaka and S.
Masunaga,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Hypoxia and glucose deprivation
have been suggested to play important roles in resistanceto radiation [1]. Attempts to sensitize tumor cells by exploiting the tumor microenvironment have been studied.
A major mediator of the cellular hypoxic response, hypoxia inducible factor 1 (HIF-1), is a potential target forcancer therapy, because it transcriptionally regulates anumber of genes, including those involved in glucose
metabolism, angiogenesis and resistance to chemotherapy
and radiation therapy [2]. We previously reported that thedisruption of Hif-1α enhanced the sensitivity of murine
squamous cell carcinoma (SCC-VII) cells to gamma-ray[3]. In the present study, we investigated whether the
disruption of Hif-1α affects the radiosensitivity of
SCC-VII cells to the boron neutron capture reaction(BNCR). Previous studies reported that HIF-1 is likely
involved in DNA damage and DNA repair. We first examined the extent of DNA damage after exposure to ionizing radiation or neutron beams. Furthermore, in order todetermine the intracellular 10B levels in tumor cells,
neutron-induced autoradiography was performed.
(;3(5,0(176 In order mark the sites of DNA damage signaling, we established SCC-VII cells expressing
EGFP -fused 53BP1 fragment (SCC-VII-BP1 cells).
SCC-VII-BP1 cells and SCC-VII-BP1 Hif-1α-deficient(ΔHif-1α) cell suspensions were exposed to gamma-rays(Co-60 Gamma-ray Irradiation Facility) or neutron beam
(KUR Heavy Water Facility). The irradiated cells wereseeded onto coverslips, and fixed with 4% formaldehyde.
The intracellular localization of the EGFP-BP1 proteins
was monitored by fluorescence microscopy.
In order to estimate the uptake of boron 10 (10B), neutron
autoradiography was performed using CR-39 detec-tors.
Cells grown under normoxia or hypoxia on CR-39 weretreated with BPA (60 ppm), and then fixed. CR-39
detectors were exposed to thermal neutrons at a fluencyof 3×1012 n࣭cm-2 (60 min), and etched in 6 N NaOH
solution at 70Υfor 45 min. The etched pits were counted
using light microscope.

tion- or neutron beams-induced DNA damage. We firsttested whether the BP1 foci can be detected in the
SCC-VII-BP1 cells. It was found that the number of fociafter gamma irradiation was formed in a dose dependent
manner (Fig 1A). Next, SCC-VII-BP1 cells and
SCC-VII-BP1 ΔHif-1α cells were cultured under
normoxic or hypoxic condition, incubated with BPA, andthen exposed to neutron beams. As shown in Fig. 1B,
fewer 53BP1 foci occurred in SCC-VII-BP1 (hypoxia)
cells than in SCC-VII-BP1 (normoxia) cells. On the other
hand, the number of foci did not differ significantly in
SCC-VII-BP1 ΔHif-1α cells (hypoxia and normoxia).

(A)

(B)

Figure. 1: (A) The number of BP1 foci 60 min after gamma
irradiation. (B) The number of BP1 foci 30 min after neutron
beam irradiation. The cells were exposed to neutrons at a fluency of 4.01011 n࣭cm-2.

We also examined whether the disruption of Hif-1α affects the uptake of BPA by calculating he average tracks
on CR-39 per cell. The average tracks per cell were 3.5
tracks for SCC-VII (normoxia) cells and 1.8 tracks for
SCC-VII (hypoxia) cells, suggesting that BPA was accumulated in SCC-VII (normoxia) cells more than in
SCC-VII (hypoxia) cells. The average tracks per cellwere 4.31 tracks for SCC-VII ΔHif-1α (normoxia) cells
and 4.72 tracks for SCC-VII ΔHif-1α (hypoxia) cells. The
results indicate that, if Hif-1α is disrupted, there was little
difference in 10B concentration in normoxia-treated andhypoxia-treated cells.
5()(5(1&(6>@ S. Masunaga HWDO, Int. J. Rad. Biol.  (2016)
187–194.
>@ Z. Luo et al., Neuropharmacology. (2015)
168–174.
>@ Y. Sanada HWDO, Int. J. Rad. Biol.  (2018)
88-96.

5(68/76
53BP1 is an early participant in the DNA damage response, and a fusion protein consisting of 53BP1 and
GFP (GFP-53BP1) is used as a marker of the DNA damage response. In this study, we established SCC-VII cells
expressing EGFP-fused 53BP1 fragment, and counted thenumber of BP1 foci formed in response to ionizing radia-

31P6-12‑74‑

,352-(&75(6($5&+(63URMHFW

‑75‑

35

Project Research on Advances in Isotope-Specific Studies Using Muti-Element
Mössbauer Spectroscopy

M. SetoInstitute for Integrated Radiation and Nuclear Science,
Kyoto University
OBJECTIVES AND PERFORMED RESEARCHSUBJECTS:
The main objectives of this project research are the investigation of the fundamental properties of new materials and the development of the advanced experimental
methods by using multi-element Mössbauer spectroscopy.
One of the most irreplaceable features of the Mössbauer
spectroscopy is to extract element-specific or isotope-specific information. As the Mössbauer resonanceline is extremely narrow, hyperfine interactions are wellresolved and give us the information on the surrounding
electronic states and magnetism. Therefore, promotion of
the variety of Mössbauer isotope provides more usefuland valuable methods for modern precise materials science of complex systems, such as biological substances,multi-layer films, and complicated-structured matter.
In this project research, each group performed their research by specifying a certain isotope:
57
Fe in P8-1, P8-2, P8-3 and P8-4
119
Sn in P8-5
119
Sn and 151Eu in P8-6
197
Au in P8-7 and P8-8
Development for other isotopes in P8-9
The subjects of research are as follows:
P8-1 Analysis of iron-based products using Mössbauer
spectroscopy – iron oxide scale generated in the boiler
feed-water in thermal power plant – (Y. Akiyama et al.)P8-2 EFG tensor of Fe2+ in M2 site of orthopyroxeneby single crystal Mössbauer microspectroscopy (K.
Shinoda et al.)P8-3 Temperature dependence of Mössbauer spectra for
Fe2O3-Al2O3 solid solution (S. Takai et al.)P8-4 A nuclear resonance vibrational spectroscopic
study of oxy-myoglobin (Y. Yamamoto et al.)P8-5 Mössbauer spectroscopy on the antiperovskite
oxide superconductor Sr3-xSnO (Y. Maeno et al.)P8-6 Researches on magnetism in a novel Kondo lattice(Y. Kamihara et al.)P8-7 Study on structure of gold complexes coordinatedwith α-amino acids by means of 197Au Mössbauer
spectroscopy (H. Murayama et al.)P8-8 197Au Mössbauer study of supported Au
nanoparticles catalysis II (Y. Kobayashi et al.)P8-9 Development of Mössbauer spectroscopy for 166Er(S. Kitao et al.)

31P8

‑76‑

MAIN RESULTS AND CONTENTS OF THIS REPORT:
Y. Akiyama et al. (P8-1) investigated iron oxide scales
generated in the pipe of the boiler feed-water system inthe thermal power plant with oxygenated treatment. The
information of chemical components of the iron oxide
resolved by Mössbauer spectroscopy is necessary formagnetic separation system to remove the scales.
K. Shinoda et al. (P8-2) have developed Mössbauer microspectrometer and applied it to the studies of M2 site oforthopyroxene in a crystallographically-oriented enstatite
crystal. The EFG tensor of the Fe2+ at the M2 site was
successfully determined.
S. Takai et al. (P8-3) studied temperature dependence of(Fe2O3)1-x(Al2O3)x solid solutions with x = 0.5 by Mössbauer spectroscopy. The temperature dependence of thespectra apparently showed a spectral change due to thermally distributed spin interaction with an effect of small
particle size.
T. Ohta and Y. Yamamoto et al. (P8-4) have been investigating on oxymyoglobin through vibrational studies toreveal the relationship between the function and the conformation of Fe-O2 bond in oxymyoglobin.
Y. Maeno et al. (P8-5) studied antiperovskite oxide superconductors Sr3-xSnO. Temperature dependence of119
Sn Mössbauer spectra of Sr3-xSnO (x Ң0.5) have revealed the presence of Sn4- site and a site of Sn4hole-doped by Sr deficiency.
Y. Kamihara et al. (P8-6) have studied magnetic phases
in novel Kondo Lattice, EuSn2As2 though 151Eu and 119Sn
Mössbauer spectroscopies. Temperature dependences
clearly showed the magnetic splitting below 20K both in
Eu and Sn spectra.
H. Murayama et al. (P8-7) investigated gold complexes
coordinated with amino acids by 197Au-Mössbauer spectroscopy and obtained the characterization of Au(III) andAu(I) components. This information is helpful for producing Au nanoparticles deposited on various supports.
Y. Kobayashi et al. (P8-8) applied 197Au-Mössbauer
spectroscopy to the studies on Au nanoparticles catalysis
supported with Hydroxyapatite. The comparison of thecatalysis prepared by several calcination temperatures
showed a slight effect by this treatment.
S. Kitao et al. (P8-9) have developed Mössbauer sources
for several less-common Mössbauer spectroscopy. As forsource materials of 166Er-Mössbauer spectroscopy, improvement of source activity in HoAl2 was successfully
confirmed. This source is useful for various researches
for Er compounds.

35

Analysis of Iron-based Products Using Mössbauer Spectroscopy- Iron Oxide Scale Generated in the Boiler Feed-water in Thermal Power Plant -< $NL\DPD0+LUDPDWVX.$NL\DPD)0LVKLPD
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0 6HWR
Graduate School of Engineering, Osaka University
Department of Nuclear Technology and Applied
Engineering, Fukui University of Technology
2National Institute for Materials Science
3
Shikoku Research Institute Inc.,
4
Ebara Industrial Cleaning Co., Ltd.,
5
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
1

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VFDOH EHFDXVH D SDUW RI WKH SDUDPDJQHWLF SDUWLFOHV ZHUHFDSWXUHG HYHQ LQ WKH VHSDUDWLRQ FRQGLWLRQV WKDW WKH SXUHSDUDPDJQHWLFSDUWLFOHVFDQQRWEHFDSWXUHG%DVHGRQWKHUHVXOWV ZH DUH FXUUHQWO\ GHVLJQLQJ +*06 V\VWHP IRUUHPRYLQJWKH27VFDOH

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WKHWKHUPDOSRZHUJHQHUDWLRQ>@3

‑77‑

REFERENCES:>@ 0+LUDPDWVXet al.-3K\V&RQI6HU1293 35

EFG tensor of Fe2+ in M2 site of orthopyroxene bysingle crystal Mössbauer microspectro-scopy

K. ShinodaDQGY. Kobayashi
'HSDUWPHQWRI*HRVFLHQFHV*UDGXDWH 6FKRRO RI 6FLHQFH2VDND&LW\8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 57Fe Mössbauer spectroscopy has
been widely used for the analysis of Fe in Fe-bearing
minerals. Powdered mineral is generally used as a Mössbauer sample, in spite of the usefulness of the conventional method, it is not useful for the Mössbauer analysisof any narrow area in a crystal or mineral grain. To
overcome the disadvantage of spatial resolution by powder method, several Mössbauer microspectrometers havebeen proposed. Mössbauer microspectroscopy will be
widely used for measuring spectra of a grain in a thinsection in future. Intensities of component peaks in aquadrupole doublet of a thin section as a single crystal
are asymmetric and vary depending on the angle between
the direction of incident γ-rays and the crystallographic
orientation of the thin section. Intensity of quadrupole
doublet (,K / ,WRWDO ) means a ratio between area of the peakof the higher energy (,K) and total area of the doublet(,WRWDO=,K +,O) (sum of ,K and area of the lower energy (,O)).
The intensity of component peaks of a 57Fe Mössbauer
doublet is related to an electronic field gradient (EFG)
tensor of the site containing Fe2+ and Fe3+ (Zimmermann,
1975 and 1983). Thus, EFG determination is important in
Mössbauer measurements of thin section as a single
crystal. Zimmermann (1975, 1983) introduced experimental determination of EFG tensor from the Mössbauer
spectrum of a single crystal, and proposed a formulationof the EFG tensor from the intensities of the component
peaks of asymmetric Mössbauer doublet.
In pyroxene, Fe2+ in 01, Fe2+ in 02 and Fe3+ in 01
sites are possible. As three doublets overlap in Mössbauer spectrum of pyroxene, it is important to reveal EFG ofthree doublets to analyze Mössbauer spectrum of pyroxene thin section. Tennant HWDO. (2000) revealed the EFG
tensor of Fe2+ at the octahedral 01 site of clinopyroxene.
Shinoda and Kobayashi (2019) revealed EFG the tensor
due to Fe3+ in 01 site of clinopyroxene. In this study,
Zimmermann's method was applied for single crystal
57

Fe Mössbauer spectra of a enstatite crystal on oriented
thin sections to determine the EFG tensor of Fe2+ at the02 site of 3EFD orthopyroxene of orthorhombic crystal
system. Chemical formula of this sample was (Mg2.03,
Fe0.16)(Si1.78, Al0.13)O6 by EDS analyses.

3

‑78‑(;3(5,0(176 DQG 5(68/76 A single crystal ofenstatite from Turiani, Morogoro, Tanzania was used forthis study. Three crystallographically oriented thin sections which are perpendicular to a*, b* and c* were prepared by measuring X-ray diffraction using precession
camera. Nine Mössabuer spectra of oriented thin sections
were measured. In this study, Cartesian coordinate (X Y
Z) is set as X//c*, Y//a*, Z//b*, where a*, b*, c* are reciprocal lattice vectors of enstatite. Mössbauer measurements were carried out in transmission mode on a constant acceleration spectrometer with an Si-PIN semiconductor detector (XR-100CR, AMPTEK Inc.) andmulti-channel analyzer of 1024 channels. A 3.7GBq
57
Co/Rh of 4mmφ in diameter was used as γ-ray source.
An 57Fe-enriched iron foil was used as velocity calibrant.
The two symmetric spectra were folded and velocity
range was ±5mm/s. Thickness corrections of raw spectra
were not done.

Fig.1 shows representative Mössbauer specrtum of enstatite measured under incident γ-ray parallel to a*-axis. A
doublet due to Fe2+ in M2 site of orthopyroxene was observed. Isomer shift, Q-splitting, and line width were1.06 2.11 and 0.34 mm/s, respectively. From nine sets ofintensity of quadrupole doublet, three components oftraceless tensor were calculated as 0.116, -0.045 and-0.075. Asymmetric parameter η was 0.266.
REFERENCES>@ 5Zimmermann (1983) Advances in Mössbauer
spectroscopy (Thosar, B.V. Ed.). pp.273-315, Elsevier Scientific Publishing Co. Amsterdam.
>@ 5Zimmermann (1975) Nucl. Instr. and Meth. 128,
543.
>@ :&Tennant, & $ McCammon and 5 Miletich(2000) Phys. Chem. Min., , 156-163.
>@ .Shinoda < Kobayashi (2019) J. Min. Petro.Sci.,
114, 130-141

35

7HPSHUDWXUH'HSHQGHQFHRI0|VVEDXHU6SHFWUDIRU)H2$O26ROLG6ROXWLRQS. Takai1, H. Nakaishi1, K. Ota1, T. Yabutsuka1, T. Yao2,
S. Kitao3, M. Seto3*UDGXDWH6FKRRORI(QHUJ\6FLHQFH.\RWR8QLYHUVLW\.\RWR8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Although both Į-Fe2O3 andĮ-Al2O3 possess corundum-type structure, the solid solution range is so restricted as approximately 10 % from theterminal compositions due to 5.6 % smaller F-length for
Al2O3 in comparison with Fe2O3 [1]. We have recently
revealed that corundum-type structured solid solution canbe obtained in the hole compositional range of Fe2O3–
Al2O3 system by means of mechanochemical method
using high-energy ball milling technique. In terms ofthe continuous substitution of non-magnetic aluminum
ions instead of iron in Fe2O3, dilution of spin interaction
can be achieved in corundum-type structure, which
would result in the variation of magnetic properties of(Fe2O3)1-x(Al2O3)x solid solution system.
Į-Fe2O3 exhibits antiferromagnetic properties at low
temperatures, which undergo Morin transition at 265 K
on heating to show a weak ferromagnetic. In the previous study (30121), Mössbauer spectroscopy experiments
have been carried out on (Fe2O3)1-x(Al2O3)x solid solutions at room temperature. It is found that the Mössbauer spectra varies from sextet peaks at x = 0 into almost doublet at x = 0.50. This indicates that substitution of aluminum ions allows the change in magnetic
properties from weak ferromagnetism to paramagnetic
state by reducing the spin interactions. It is also expected that spin ordering would be attributed by temperature, i.e. the Mössbauer spectra should be altered by
reducing temperature. In the present study, we measured the Mössbauer spectra in the temperature range from4 K up to the room temperature to investigate the variation of magnetic properties of (Fe2O3)0.5(Al2O3)0.5.

apparent doublet peaks are observed as the previous investigation of last year (30121). The doublet diminisheswith decreasing temperature, while the sextet grows
around 200 K, and almost sextet peaks are remained below 40 K. It is supposed that spin interaction thermally
disturbed and attributed by small particle size would
bring about the ordering at lower temperatures. Further
precise analysis is now carried out accompanied by theneutron diffraction. Moreover, additional low temperature Mössbauer experiments are planning with othercompositions.

300 K

200 K

Transmission / arb. units

100 K

77 K

40 K

20 K

10 K

(;3(5,0(176 Stoichiometric mixture of J-Fe2O3
and J-Al2O3 reagents were put into a silicon nitride milling pod with 10 milling balls with the diameter of I10.
In the present study, the compositions were selected as x
= 0.50 for (Fe2O3)1-x(Al2O3)x system. Mechanical alloying has been carried out using a planetary ball millingmachine operated at 800 rpm for 240 min. The crystalline phase of the obtained sample was confirmed by
X-ray diffraction.
For the measurement of Mössbauer spectroscopy, 57Co
in Rh was employed as the J-ray source. Doppler velocity scale has been calibrated by using Fe foil. The
Mössbauer spectra were collected at various temperatures
below 300K. Low temperature has been achieved byusing He gas flow type refrigerator or liquid N2 cryostat.

-15

-10

-5

0

5

10

15

-1

Velocity / mm兟s

Fig. 1 Temperature dependence of Mössbauer spectrafor (Fe2O3)0.5(Al2O3)0.5.

5()(5(1&(6[1] A. Muan HW DO, - $P &HUDP 6RF, 39 (1956)
207-214.
[2] S. Takai HWDO, 6ROLG6WDWH,RQLFV, 313 (2017) 1-6.

5(68/76 The Mössbauer spectra measured at various temperatures are represented in Fig. 1. At 300 K,

31P8-3‑79‑

35

$1XFOHDU5HVRQDQFH9LEUDWLRQDO6SHFWURVFRSLF6WXG\RI2[\0\RJORELQ

T.Ohta,T. ShibataM. SaitoM. SetoY. KobayashiS. YanagisawaT. Ogura Y. Yamamoto S. Neya and
A. Suzuki

'HSDUWPHQWRI$SSOLHG&KHPLVWU\)DFXOW\RI(QJLQHHU
LQJ6DQ\R2QRGD&LW\8QLYHUVLW\
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8QLYHUVLW\*UDGXDWH6FKRRORI/LIH6FLHQFH8QLYHUVLW\RI+\RJR
*UDGXDWH6FKRRORI3KDUPDFHXWLFDO6FLHQFHV&KLED8QLYHUVLW\'HSDUWPHQWRI0DWHULDOV(QJLQHHULQJ
1DWLRQDO,QVWLWXWHRI7HFKQRORJ\1DJDRND&ROOHJH

5(68/76 Based on the 57Fe PVDOS of the proteins(Figure 2A), we found that the vibrational spectrum ofMbO2(Proto) can be better reproduced by the spin polarized Fe3+-O2– state calculated on the basis of broken-symmetry singlet state, rather than the Fe2+-O2
closed-shell singlet one, in terms of the vibrational energies and peak intensities of the major bands due to the
Fe-O2 bond and the bonds between heme Fe and pyrrole
nitrogen atoms. This finding supported the dominance ofthe Weiss form1 in the nature of the Fe-O2 bond in theprotein.

,1752'8&7,21 Myoglobin (Mb), an oxygen (O2)storage hemoprotein, has been served as a paradigm forthe structure-function relationship of metalloproteins. O2
is reversibly bound to a ferrous heme Fe atom (Fe(II)) in
Mb. Although the reaction between O2 and heme Fe(II)of Mb is often considered as one of the simplest biological reactions, in fact, the reaction is much more complicated than it appears. Upon oxygenation of the protein,ground state triplet O2 is bound to a high-spin quintet
heme Fe(II) in Mb to yield a low-spin singlet heme Fe(II)in oxy Mb (MbO2), which is considered as a mixture of
Weiss (Fe3+(6 = 1/2)-O2–(6 = 1/2)),1 Pauling (Fe2+(6 =0)-O2(6 = 0)),2 and McClure forms (Fe2+(6 = 1)-O2(6 =1))3. We characterized MbO2s possessing 57Fe-enrichedheme cofactors (Figure 1) using nuclear resonance vibrational spectroscopy (NRVS) to elucidate the electronic
nature of the Fe-O2 bond.4
Figure 2. 57Fe PVDOS of MbO2(Proto) at 43 K (bottom),MbO2(Meso) at 27 K (middle) and MbO2(7-PF) at 26 K
(top) (A), expanded 57Fe PVDOS of MbO2(Proto) (solidline), MbO2(Meso) (dotted line) and MbO2(7-PF) (brokenline) in 0–100 cm–1 (B), and deconvolution of Fe-O2 band
region, 370–470 cm–1, of MbO2(Proto) (C).

Figure 1. The structures andnumbering system for theheme cofactors used in the
study. Proto (R2 = R7 = CH3,R3 = R8 = CH=CH2), Meso (R2= R7 = CH3, R3 = R8 = C2H5),
and 7-PF (R2 = CH3, R3 = R8 =C2H5, R7 = CF3).

(;3(5,0(176 Iron-57Fe (95 atom%, Merck) wasused to prepare 57Fe-enriched heme cofactors. Spermwhale Mb was purchased as a lyophilized powder from
Biozyme and used without further purification. Apoprotein of Mb was prepared using the procedure of Teale5.
57
Fe-enriched Proto, Meso, and 7-PF (Figure 1) wereincorporated into apoprotein, and then the obtained proteins were converted to oxy forms, i.e., MbO2(Proto),
MbO2(Meso), and MbO2(7-PF), respectively, using thestandard procedure. NRVS measurements were performed at SPring-8, BL09XU6. During the data collection,
the protein samples were maintained at low temperatureusing a liquid He cryostat (head temperature <10 K).
Spectra were recorded between -20 and 80 meV in 0.25
meV steps. 57Fe partial vibrational density of states (57Fe
PVDOS) was calculated using a program PHOENIX7.

31P8-4‑80‑

The comparison of the 57Fe PVDOS below 100 cm–1
between the proteins (Figure 2B) indicated that translational motion of heme cofactor is larger in MbO2(Proto)compared with those in MbO2(Meso) and MbO2(7-PF).
The large conformational flexibility of MbO2(Proto)
would be due to the presence of multiple conformationsof the Fe–O2 bond, because deconvolution of the Fe-O2
band region of the 57Fe PVDOS of MbO2(Proto), i.e.,
400-430 cm–1, yielded at least three peaks at 402, 421 and436 cm–1 (Figure 2C), indicative of the presence of multiple conformations.
5()(5(1&(6[1] J. J. Weiss, 1DWXUH, , 83-84 (1964).
[2] L. Pauling, 1DWXUH, , 182-183 (1964).
[3] D. S. McClure, 5DGLDWLRQ5HV6XSSO, , 218-242 (1960).
[4] T. Ohta HWDO, %LRFKHPLVWU\, , 6649-6652 (2018).
[5] F. W. J. Teale, %LRFKLP%LRSK\V$FWD, , 543 (1959).
[6] Y. Yoda HWDO., +\SHUILQH,QWHUDFW, , 83-86 (2012).
[7] J. T. Sage HWDO., -3K\V&RQGHQV0DWWHU, í7722 (2001).

35

Mössbauer spectroscopy on the antiperovskite
oxide superconductor Sr3−xSnO

Y. Maeno, M. Seto1, S. Kitao1, S. Yonezawa, A. Ikeda,
S. Koibuchi, and M. Oudah, 2
Graduate School of Science, Kyoto University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Stewart Blusson Quantum Matter Institute, University of
British Columbia
INTRODUCTION:
Antiperovskite (inverse perovskite) oxides A3BO (A: group-2 element, B: group-14
element) crystalize in the same structure as the ordinary
perovskite oxides, but with inverted positions of the cations and anions [1]. In those materials, a metallic anion
B4− (Sn4−, Pb4−, etc.) is expected to satisfy the charge
neutrality, assuming the ionic states of A2+ and O2−. Metallic anions are rare especially in oxides. Originatingfrom the unusual oxidation state, antiperovskite oxides
are candidates for topological crystalline insulators [2, 3].
In 2016, some of the present authors discovered the firstsuperconductor among antiperovskite oxides, Sr3−xSnO[4]. Reflecting the nontrivial topology in the normal state,
topological superconductivity is theoretically possible inthis compound [5]. To investigate the unusual propertiesof this material, we performed Mössbauer spectroscopyon the Sn nucleus.
EXPERIMENTS: The sample was prepared from Sr(Sigma-Aldrich, 99.99%) and SnO (Sigma-Aldrich
99.99%) using the reaction (3−x)Sr + SnO Ѝ Sr3−xSnO,
with a condition of x ~ 0.5 [6]. From powder x-ray diffraction, we confirmed that the sample is dominated by
Sr3−xSnO. Superconductivity with a volume fraction of
about 10% was observed below 5 K in a magnetization
measurement. We also observed superconductivity ofβ-Sn impurity. From the diamagnetic signal, we estimatedthe amount of β-Sn impurity to be 14 mol %. We conducted Mössbauer spectroscopy at the Institute forFig. 1. Mössbauer spectra of Sr3−xSnO (x ~ 0.5) with respect to the isomer shift of BaSnO3. Each spectrum isshifted upward by 0.1 for visibility. γ-ray absorption with
an isomer shift similar to that of Mg2Sn evidences presence of Sn4−. In addition, another absorption with a larger
isomer shift originating from Sr deficiency was observed.

Integrated Radiation and Nuclear Science, Kyoto
University. 119mSn in the form of CaSnO3 (Ritverc GmbH,
740 MBq) was used as the γ-ray source.
RESULTS: We present the Mössbauer spectra of
Sr3−xSnO in Fig. 1. We observed a clear γ-ray absorption
with a shoulder at high temperatures, and the relative
intensity of the shoulder increases at low temperatures.
To analyze the data, we fitted the spectra with three Lorentz functions, corresponding to the main and shoulder
absorptions as well as β-Sn impurity. The isomer shift
and intensity of one of three Lorentzians were fixed tothat of the reported value for β-Sn and 14%, respectively.
As a result, the isomer shifts at 3 K are fitted to be
1.960(6) mm/s for the main absorption and 2.973(11)mm/s for the shoulder. Since the isomer shift of the main
absorption is close to that of Mg2Sn, in which Sn4− isanticipated, this result evidences presence of Sn4− in

Sr3−xSnO. The shoulder with a larger isomer shift originates from a modified ionic state of Sn4− hole-doped bySr deficiency. The greater temperature evolution of theshoulder, corresponding to a higher local Debye temperature, is consistent with the Sn atoms neighboring the Srvacancies.
Detailed results were published in Ref. [6], where weevaluated the isomer shift and the Debye temperatureusing the first-principles calculation.
REFERENCES:[1] A. Widera and H. Schafer, Mater. Res. Bull. 15 (1980)
1805–1809.
[2] T. Kariyado and M. Ogata, J. Phys. Soc. Jpn. 80(2011) 083704.
[3] T. H. Hsieh et al., Phys. Rev. B 90 (2014) 081112(R).
[4] M. Oudah et al., Nat. Commun. 7 (2016) 13617.
[5] T. Kawakami et al., Phys. Rev. X 8 (2018) 041026.
[6] A. Ikeda et al., Phys. Rev. B 100 (2019) 245145.

31P8-5‑81‑

35

Researches on magnetism in a novel Kondo lattice
Relative transmission(kcounts)
㻌Y. Kamihara, R. Sakagami, S. Kitao1, M. Seto1
Department of Applied Physics and Physico-Informatics,
Keio University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University

EXPERIMENTS: Synthesis procedure of the polycrystalline undoped EuSn2As2 has been reported in ref.[6].
Optical systems for the M|ssbauer spectroscopy areconventional.[7]RESULTS: As shown in Fig. 1, M|ssbauer spectra of151
Eu demonstrate a clear magnetic splitting at T = 4.2 K
for undoped EuSn2As2. As shown in Fig. 2, the 119Sn
M|ssbauer spectra also demonstrate magnetic splitting at
T < 20 K. A quantitative analysis on internal magnetic
field should be performed in the collaborative research in2020.

31P8-6

‑82‑

30 K

94
92
90
88

4.2 K

-50

0
50
-1
Velocity (mm s )Fig. 1. 119Eu Mössbauer spectra for polycrystalline
undoped EuSn2As2.

1.00
30 K

0.95
0.90
0.85
1.00

20 K

0.95

Relative transmission

INTRODUCTION: In this research, we demonstrate
the magnetic phases in a novel Kondo lattice, EuSn2As2.
EuSn2As2 is an inter-metallic compound, which is reported by Arguilla et al.[1] and is a 2 dimensional layered
magnetic compound composed by Eu cation and negative
charged Sn2As2. In a unit cell of EuSn2As2, van der Waals
interaction is dominant force to make chemical bonding
along c-axis. Such characteristic chemical bonds are similar to those of "state of art" 2 dimensional topologicalinsulator, Bi2(Se, Te)3 [2,3,4], which have been focusedas thermo electric materials since 1961 or earlier. In 2019,
we unveiled a complex magnetic phases in EuSn2As2.
In undoped EuSn2As2, density functional theory (DFT)demonstrates that a sublattice of Eu orders
antiferromagnetically at temperature (T) = 0 K, although
Eu ions ferromagnetically ordered along a / b axes; i.e.
the Eu orders ferromagnetic intra layer.
In 2019, we demonstrated spontaneous magnetic moments of undoped EuSn2As2 using DC-magnetic momentmeasurements. The spontaneous magnetic moments verify a ferromagnetic phase of undoped EuSn2As2 under
weak finite magnetic fields at low T.[5]These results indicate that a magnetic phase of undoped
EuSn2As2 is changed to the ferromagnetic order underfinite magnetic fields from the antiferromagnetic orderunder a zero field. In the ferromagnetic order phase, theEu ion exhibits ~5 PB at T < ~20 K. The magnetic moment of Eu is smaller than that of representative Eu2+.
The small magnetic moment of Eu suggests a highly
hybridized electronic orbital among Eu and Sn atomic
orbitals, although direct measurements of internal magnetic fields have not been reported for EuSn2As2.
In this research, we have measured 151Eu and 119Sn
M|ssbauer spectroscopy, and demonstrate an appearance
of internal magnetic fields at low T in undoped
EuSn2As2.

43
42
41
40

0.90
0.85
1.00
0.95

10 K

0.90
0.85
1.00
0.95

4.2 K

0.90
0.85
-10

0

10
-1

Velocity (mm s )Fig. 2. 119Sn Mössbauer spectra for polycrystalline
undoped EuSn2As2.
REFERENCES:[1] M. Q. Arguilla, et al., Inorg. Chem. Front. 4, 378-386(2017).
[2] C. L. Kane and E. J. Mele, Phys. Rev. Lett. 95,
146802 (2005).
[3] H. Zhang, et al., Nature Phys. 5, 438-442 (2009).
[4] H. J. Goldsmid and R. T. Delves, G.E.C. Journal 28,
102 (1961).
[5] K. Hirata, et al., "Spontaneous magnetic polarizationof a layered hexagonal compound, EuSn2As2", The 6thJapan-Korean International Symposium on Materials
Science and Technology (JKMST2019), Sapporo, Japan: 26th August 2019.
[6] R. Sakagami, et al., Mater. Sci. Tech. Jpn. 55, 72-76(2018). In Japanese[7] S. Kitao, et al., J. Phys. Soc. Jpn. 77, 103706 (2008).

35

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Ishida3, D. Kawamoto4 and M. Tokunaga'HSDUWPHQWRI&KHPLVWU\.\XVKX8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
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sition of 197Au, was prepared by neutron irradiation of
isotopically enriched 196Pt metal at the Kyoto University
Reactor. 7KHȖ-ray source and the samples were cooled toa temperature below 20K. The isomer shift (,6) of Au foil
was referenced to 0 mm/s. ,1752'8&7,21  Gold nanoparticles show catalytic
activities when their sizes were less than 5 nm. We havereported a simple and easy impregnation method for the
preparation of small gold nanoparticles deposited on various supports [1]. A gold complex coordinated with
ȕ-alanine (Au–ȕ-ala) was synthesized as a chloride-free
and water-soluble precursor for this method. A molecular
structure of Au–ȕ-ala was determined as mononuclear
complexes of Au3+ with square-planar coordination bymeans of in situ X-ray absorption fine structure, TG-DTA,
and DFT calculations (Fig. 1). Recently, the gold complexes coordinated with various kinds of amino acids
were synthesized to realize better precursor thanAu–ȕ-ala. In this study, the structures of the gold complexes were analyzed by 197Au Mössbauer spectra.

top view

5(68/76 As shown in Fig. 2a, the 197Au Mössbauer
spectrum for Au–ȕ-ala, which consisted of doublet peaks,
was analyzed and then the ,6 and the quadrupole splitting(46) were obtained as 4.29 mm/s and 4.93 mm/s, respectively. Similar values were obtained from analyses of thespectra for Au–GABA, Au–DAVA, and Au–EAHA. The
values of ,6–46 were in the range of data given by various four-coordinate gold(III) compounds [2]. In addition
to the doublet as same as that in the spectrum for
Au–ȕ-ala, another doublet was observed in the spectrum
for Au–Trp (Fig. 2b). The values of ,6 and 46 were 3.44mm/s and 7.83 mm/s, respectively. The characteristic
double doublets were also observed in the spectra for
JROGFRPSOH[HVFRRUGLQDWHG ZLWK Į-amino acid (His andTyr) indicating that those gold complexes were mixturesof gold(III) and gold(I).

side view

(a)
H
O

Au

N

C

Fig. 1. The geometry of Au–ȕ-ala optimized
by DFT calculation.

(b)(;3(5,0(176 Gold complexes coordinated withDPLQR DFLG ȕ-ala Ȗ-aminobutyric acid (GABA),
į-DPLQRYDOHULF DFLG '$9$  İ-aminocaproic acid
(EAHA), tryptophan (Trp), histidine (His), and tyrosine(Tyr)) were synthesized as follows: ethanol was added toa NaOH aqueous solution in which amino acid was dissolved. The amino acid solution was then added to the
HAuCl4 ethanol/water mixed solution. The mixed solution was left at –18°C for 12 h. The precipitates werecollected and washed with ethanol/water. The solid was
dried to obtain Au–amino acid complex powder [1].
197
Au Mössbauer spectra of the synthesized Au–aminoacid complexes were collected at Institute for Integrated
Radiation and Nuclear Science, Kyoto University. The
Ȗ-ray source (197Pt) feeding the 77.3 keV Mössbauer tran-

Fig. 2. 197Au Mössbauer spectra for(a) Au–ȕ-ala and (b) Au–Trp.

5()(5(1&(6>@ H. Murayama HWDO, J. Catal., (2017) 74-80.
>@ R. V. Parish, Gold Bull.,  (1982) 51-63.

31P8-7‑83‑

$X0|VVEDXHUVWXG\RIVXSSRUWHG$XQDQRSDUWLFOHVFDWDO\VLV,,

(;3(5,0(176 The supported Au nanoparticles catalysis was prepared by the deposition precipitation
method and calcination. The mixed solution of HAuCl4and HAp was kept on pH 9 and 65qC, thus the Au ionsAfterwere precipitate on HAp as Au(OH)3.
precipitation, the specimens were washed with distilledwater, and dried. These specimens were calcined for 4
hours at 200~800qC in air. At that time, Au(OH)3 was
degraded into Au metal, and the Au nanoparticles werefirmly fixed on HAp.
197

Au Mössbauer measurement was conducted using a
constant-acceleration spectrometer with a NaI scintillation
counter. The 197Au J-ray source (77.3 keV) was obtained
from 197Pt (half-life; 18.3 hrs) generated by irradiation ofneutron to 98%-enriched 196Pt metal foil using KUR.
The J-ray source and samples were cooled to 16 K, and
the spectra were recorded in a transmission geometry.
The LVRPHU VKLIW YDOXH RI D JROG IRLO ZDV UHIHUHQFHG WR 
PPV

31P8-8

‑84‑

䢵䢰䢳䢸

200°C

䢸

䢵䢰䢳䢶

䣺䢳䢲

,1752'8&7,21 The normal surface of metallic
gold does not adsorb small molecules like hydrogen andoxygen; thus, gold is not generally considered as a good
catalyst. Small particles have many edges, corners, andmetastable surfaces, and they are different from bulk forcatalytic activities. Dispersing the small particles on
supports, the catalytic activity of gold increases. Au
small particles supported on some materials show highcat-alytic activity to oxidize CO to CO2 at temperatures as
low as 197K [1,2].
The interaction between particles and supports may
give new activity to the catalysts.
Hydroxyapatite(HAp) is known as bone mineral, and it is nature friendly.
Further-more, it is good support for nanoparticles [3].
HAp binds strongly with Au, and it avoids the fusion of
the nanopar-ticles. This binding with HAp may change
the charge of Au, which is expected to show different
properties from the bulk.
We have studied the supported Au nanoparticles catalysis using 197Au Mössbauer spectroscopy.
We canobserve the signals from Au atoms without disturbancefrom sup-ports by 197Au Mössbauer spectroscopy.
Moreover, it is sensitive to the electronic states of Au
atoms.
Thus, Mössbauer spectroscopy is powerful forthe study of sup-ported catalysts.

䢵䢰䢳䢴
䢵䢰䢳䢲
䢵䢰䢲䢺
䢻䢶䢲

䢻䢵䢲

500°C

䢵

'DOLDQ,QVWLWXWHRI&KHPLFDO3K\VLFV&KLQHVH$FDGHP\
RI6FLHQFHV䣺䢳䢲

1䣅䣱䣷䣰䣶䣵,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\

5(68/76
Figure 1 shows the 197Au Mössbauer
spectra of the Au nanoparticle catalysis prepared byseveral calci-nation temperatures. All observed spectra
show almost the same shape and peak position. This
result indicates that the electronic states of thenanoparticles are nearly the same as that of metallic bulk
Au. However, in detail, the value of the isomer shiftslightly changes from 0.09 mm/s to 0.04 mm/s from the
200°C calcined sample to the 800°C calcined sample.
The direction of this change is the di-rection in which
the charge of the Au atom decreases; how-ever, thedifference is only slightly above the error, and further
verification is necessary.

䢻䢴䢲

䢴䢰䢵䢲
䢸

Y Kobayashi, J Wang1 and M Seto

䣺䢳䢲

35

800°C

䢴䢰䢴䢺

䢴䢰䢴䢸

䢯䢷

䢲

䢷

䢳䢲

䣘䣧䣮䣱䣥䣫䣶䣻䢢䢢䣯䣯䢱䣵

Fig. 1 197Au Mössbauer spectra of Au nano-particles catalysis prepared by several calcination temperatures.
The measurement temperature was 16K.

5()(5(1&(6[1] M. Haruta, T. Kobayashi, H. Sano and N. Yamada,
Chem. Lett.,  (1987) 405.
[2] M. Haruta, N. Yamada, T. Kobayashi and S. Iijima, J.
Catal.,  (1989) 301.
[3] Yanjie Zhang, Junhu Wang, Jie Yin, Kunfeng Zhao,
Changzi Jin, Yuying Huang, Zheng Jiang, and Tao
Zhang, J. Phys. Chem. C,  (2010) 16443-16450.

35Development of Mössbauer Spectroscopy for 166Er

S. Kitao1, M. Kobayashi1, T. Kubota1, M. Kurokuzu1, H.
Tajima2, and M. Seto1

method from Ho and Al. The obtained HoAl2 powder wassealed in polypropylene capsule with polystyrene resin.
The neutron irradiation has been done by the pneumatictube station(Pn) at KUR.
Since HoAl2 has a Curie temperature of about 25 K[1,2],
the source temperature had better to be kept above 40 K
to avoid line broadening by magnetic splitting. Since therecoilless fraction of Er compounds is low at high temperature, the sample and the source were usually cooledat the temperature of 40 K by using He-closed-cycle refrigerator. The gamma-rays with the energy of 80.6 keV
have been measured by CeBr3 scintillation detector.
Until last year, several 166Er experiments have alreadybeen performed at KUR by users from other researchgroups[3]. However, because of the limitation from radiation safety regulations, the radioactivity of 166Ho waslimited to 20 MBq. Some experiments had suffered frompoor statistics. Therefore, in order to promote the 166Er
experiments, we requested to extend the limitation and it
was approved to be extended to 500 MBq.
In order to check the effectiveness of the gain of source
activity and the radiation safety of experimental condition,
a comparison was done using Er2O3 absorber with thesame source material of HoAl2 at about 18 to 20 K. The
obtained activity was controlled by irradiation time. Similar measurements have been performed by 20 MBq and
98 MBq source as shown in Fig.1 and Fig.2, respectively.
The experiment was successfully performed without any
problem in radiation safety. The statistics of the spectra
was well improved by the gain of radioactivity. The results showed the improvement of the 166Ho source was
successful. The observed Mössbauer spectra showed theline broadening due to magnetic splitting of HoAl2 below
Curie temperature. This source will be useful for various
application in Er compounds, when measured at 40 K.

1

Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Graduate School of Science, Kyoto University

INTRODUCTION:
The Mössbauer spectroscopy is one of the most powerful methods for investigation of electronic states, magnetic properties, chemical properties, and so on. A remarkable feature of this method is to extract the information of the specific isotope. Although about one hundred of Mössbauer energy levels are known, research
activities in Mössbauer studies so far are quite limited,
except 57Fe and 119Sn. It is partly because commerciallyavailable sources at present are only 57Co and 119mSn for
the Mössbauer spectroscopy of 57Fe and 119Sn, respectively.
On the contrary, at the Institute for Integrated Radiation
and Nuclear Science, various short-lived isotopes can beobtained by neutron irradiation at Kyoto University Research Reactor(KUR). Moreover, some short-lived isotopes can be complementarily produced by high-energy
Ȗ-ray irradiation at the electron linear accelerator(KURNS-LINAC). Thus, we have already been performing Mössbauer spectroscopy with various isotopes(by source nuclides in parentheses): 61Ni(61Co),
125
Te(125mTe), 129I(129Te,129mTe), 161Dy(161Tb), 166Er(166Ho),169
Tm(169Er), 170Yb(170Tm), 197Au(197Pt), etc.
The main purpose of this research is to develop effective
Mössbauer sources for various isotopes and to apply thisspectroscopy to many fields of researches. Among theseresearches, an improvement of 166Er Mössbauer spectroscopy is described in this report.

REFERENCES:

EXPERIMENTS AND RESULTS:
Although several levels are known in the Mössbauer
spectroscopy of Er, the 80.6 keV level of 166Er is the mostuseful level. Since the natural abundance of 165Ho is
100 %, by neutron irradiation of natural Ho, 166Ho with ahalf-life of 26.8 hours can be obtained for the Mössbauer
source without by-product nuclides. As for the source
material, we have synthesized HoAl2, by arc-melting[

[1] E. Munck, D. Quitmann, S. Hufner, Z. Naturforsch. 21A,
847 (1966).
[2] E. Munck, D. Quitmann, S. Hufner, Phys. Lett. 24B, 392(1967).
[3] S. Nakamura, H. Yokota, S. Kitao, Y. Kobayashi, M. Saito,
R. Masuda, M. Seto, Hyperfine Interact. 240, 75 (2019).

[













+R$O(U2.

+R$O(U2.














9HORFLW\ PPV

Fig. 1. 166Er-Mössbauer spectrum of Er3O3 at 20 K using
20MBq 166Ho source in HoAl2.


9HORFLW\ PPVFig. 2. 166Er-Mössbauer spectrum of Er3O3 at 18 K using
98MBq 166Ho source in HoAl2.

3‑85‑

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PR9-2Analysis of Localization of Boron in Root Tissues by Neutron Capture Radiography

S. Kitajima1, M. Kobayashi2 and T. Kinouchi3

ing natural boron with boron-10. Further analyses basedon the detailed boron-distribution might help understandthe molecular mechanism regarding controlling root
elongation growth.

1

Department of Applied Biology, Kyoto Institute ofTechnology
2
Graduate School of Agriculture, Kyoto University
3
Institute for Integrated Radiation and Nuclear Science,
Kyoto University(A)

INTRODUCTION: In plant primary cell walls, boron
provides a cross-link as a borate ester between apiose
residues of rhamnogalacturonan II (RG-II) in pectin [1].
Thus Borate-RG-II complex is an essential factor in theformation of the pectic network, which contributes to celladhesion or physical characteristics of plants. In fact,boron deficiency causes various physiological disorders
in plants, such as necrosis of tap roots or reduced fertility.
On the other hand, the distribution of boron within planttissues still remains unclear. In our previous analyses, it
was suggested that a large amount of boron would be
distributed in the central part and cambium of radish tap
roots. In order to study the vertical distribution of boron
in plants, we tried to analyze Arabidopsis tap roots byneutron capture radiography.

(B)

(C)

1 mm

1 mm
(D)

EXPERIMENTS: Plant material> Seeds of Arabidopsis(Arabidopsis thaliana) were germinated in the hydroponic media containing 1 mM Ca(NO3)2, 0.5 mM KH2PO4,
0.5 mM K2SO4, 1 mM MgSO4, 1.5 mM NH4NO3, 75 μM
EDTA-Fe, 46 μM H3BO3, 9 μM MnSO4, 0.8 μM ZnSO4,
0.3 μM CuSO4, and 0.8 μM Na2MoO4, and cultivated at
23°C under a 16-h light/8-h dark cycle in a
60%-humidified growth chamber.
In situ visualization of boron by neutron capture radiography> After 6 days of cultivation, seedlings were fixedwith 3% glutaraldehyde solution containing 250 mM sucrose. Chilled Arabidopsis in liquid nitrogen was sectioned at 10-μm thickness by a cryostat. The section was
mounted onto CR-39 nuclear tracker detector and irradiated with epithermal neutron for 15 min by application to
the pneumatic tube in the graphite thermal column(Tc-Pn) of Kyoto University Research Reactor (KUR).
The irradiated CR-39 was etched in 6 M NaOH solution,and the resulting etch-pits were observed under an optical
microscope.

(E)

1 mm
(F)

(G)

1 mm

RESULTS: Etch pit could be observed clearly in thevertical section of the Arabidopsis roots (Fig. 1C). As
well as radish tap roots [1], boron in Arabidopsis roots
was concentrated at the center and outer peripheral tissues as indicated by arrows. Interestingly, at the tip of
the root, high amounts of boron were observed (Fig. 1E,
G). Fig. 1D and F shows the root cap and apical meristem, which consists of undifferentiated cells (meristematic cells). Since both tissues cause cell division actively and require physical strength by synthesizing newcell walls, a large amount of boron would be applied.
Recently, we improved the resolution of this visualization
technique by culturing plants in a special solution replac-

1 mm

1 mm

Fig. 1 Detection of boron in Arabidopsis tap roots using
neutron capture radiography. (A): Stereomicroscopic image of Arabidopsis on the sixth day after seeding. Taproots applied with neutron capture radiography. (B), (D)and (F): Optical microscopic images of cross-sections ofArabidopsis roots taken before irradiation; (C), (E), and(G): etch-pit images of (B), (D), and (F) after irradiation,
respectively.
REFERENCES:[1] M. Kobayashi, T. Matoh, J. Azuma, Plant Physiol.,
110:1017–1020 (1996).

31P9-2‑89‑

PR-9-3

Improvemnt of In Situ Visualization of Boron Distributed in Plants
by Neutron Caputure Reaction

T. Kinouchi

The irradiated CR-39 plate was etched in 6 M NaOH
solution, and the resulting etch-pits were observed underan optical microscope [1].

Institute for Integrated Radiation and Nuclear Science,
Kyoto University

RESULTS: Both Fig. 1(B) and 1(D) are radiographs of
the radish tap root, which were cultured with natural boron and boron-10 including culture media respectively.
As expected, a large of etch-pits, which were generated
from boron-10 on CR-39 by boron-neutron capture reaction, were imaged as small black spots. Especially,
Fig. 1(D) showed quite a number of etch-pit which were
not equally distributed, but were concentrated at thecenter and outer peripheral tissues as indicated by arrows. To judge from the optical microscopic image ofthe original cross section (Fig. 1(C)), the outer peripheral tissues were supposed as cambium, and the vascular bundles arranged in ring shape were observed.
The concentrated formation of etch-pits was considered
as evidence for the distribution of a large numbers ofboron, indicating cell dividing actively in such tissues.

INTRODUCTION: Boron is an essential nutritional
element for all plants, however, a deficiency or an excess
of boron causes various growth disorders of them. For
all crops due to boron-toxicity which occurs frequently
all over the world, a drastic solution has not been developed, because boron analysis methods with high resolution has not yet been well-developed. We still have apoor understanding about physiological functions of boron in plants. Thus, in order to collect multidimensional
information on how much boron is localized in which
tissue/cell at any stage of growth, we are developing anin situ visualization technique capable of detecting the
localization of boron with high resolution, by applying
neutron capture radiography with a solid-state nuclear
track detector, CR-39[1,2]. On the other hand, boron
captured by neutron is only boron-10, which is a stable
isotope, and the ratio of these existing in nature is 20%.
It means that, among boron absorbed from the roots ofthe plants, their ratio visualized by neutron capture radiography is also 20% at maximum. Since the low content of boron-10 made it difficult for visualization of thelocalization of boron in the tissue of a plant, we tried toincrease the resolution by culturing the plant in a special
solution replacing natural boron with boron-10 as a nutrient.
EXPERIMENTS: Plant materials and growth conditions> Seeds of radish (Raphanus sativus L.) were seededon the moderately moisturized vermiculite and cultivatedat 23°C under a 16-h light/8-h dark cycle in a
60%-humidified growth chamber. A week later, theirseedlings were transferred to the hydroponic media containing major nutrients (1 mM Ca(NO3)2, 0.5 mM
KH2PO4, 0.5 mM K2SO4, 1 mM MgSO4, and 1.5 mM
NH4NO3) and micronutrients (75 μM EDTA-Fe, 46 μM
H310BO3, 9 μM MnSO4, 0.8 μM ZnSO4, 0.3 μM CuSO4,
and 0.8 μM Na2MoO4) under the same condition, andcultured for 10 days.
In situ visualization of boron in plants using neutron
capture radiography> Mounted slice (10-μm thickness)of the radish tap root onto CR-39 (20 mm×30 mm) was
irradiated with epithermal neutron for 15 min by applying to the pneumatic tube in the graphite thermal column(Tc-Pn) of Kyoto University Research Reactor (KUR).

(A)

(B)

(C)

(D)

Fig.1 Distribution of boron in the radish tap root. (A)and (C): Optical microscopic images of cross sections of
the radish tap root. Each root has a diameter of ~5 mm.
(B) and (D): Etch-pit images of (A) and (C) after neutronradiation, respectively.
REFERENCES:[1] M. Kobayashi and T. Kinouchi, KURRI Progress
Report 2014, 129 (2015).
[2] T. Kinouchi, KURNS Progress Report 2018, 121(2019).

31P9-3‑90‑

,352-(&75(6($5&+(63URMHFW

‑91‑

35

7KHHIIHFWRIERURQQHXWURQFDSWXUHWKHUDS\RQQRUPDOWLVVXHV

M. Suzuki,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH .\RWR
8QLYHUVLW\ 

In this research project, five research projects were included. In this summary, two research projects (P102 and P10-3) could not be reported due to unexpectedor uncontrolled events. Details of each project is referred to the following contents.
3 “The effect of boron neutron capture therapy(BNCT) on normal lung in mice.”
We have already reported the survival fraction following whole thorax irradiation with X-ray irradiation.
In 2020, the effect of thermal neutron beam at KUR on
normal lung was investigated. The mice were sorted
into four treatment groups, 40-min, 50-min, 60 min,and 70-min irradiation groups. In each group, six toseven mice were irradiated. In 40-min and 50-min irradiation groups, all the mice survived within an observation period of 40 to 140 days. In 60-min irradiationgroup, six mice died within an observation period of 12days, three mice survive within an observation periodof 140 to 180 days, and one mouse died at 146 days after
the treatment. In 70-min irradiation group, all the three
mice died within 10 days.
3 “Study of the influence on normal liver tissue by
BNCT.”The purpose of this study is to establish systematicallyand continuously technique that can analyze the harmful phenomenon in the normal liver tissue of BNCT.
Female C57BL6 mice at 6weeks of age were injected 1000mg/kg p-boronophenylalanine (BPA) solution subcutaneously 2 hours before neutron irradiation.
The mice were irradiated for 60 minutes at the 1MW
output. One week after irradiation, mice were sacrificed, and the blood and livers were analyzed. Blood
and liver boron concentrations 2 hours and 3 hours
after the administration of 1000 mg / kg BPA were
quantified using Inductively Coupled Plasma Spectrometer (ICP). The livers of the mice 6 months after
neutron irradiation were stained with Masson trichrome. HE staining and triglyceride quantification
were performed to investigate degree of the steatosis
in the mouse normal liver tissue after BNCT. Western
blotting was performed to deter- mine the expression
level of Sonic Hedgehog protein. In addition, Masson

3

‑92‑

trichrome staining was performed to determine thedegree of liver fibrosis six months after neutron irradiation.
3 “The Effect of Boron Neutron Capture Therapy
to Normal Bones in Mice.”
In this study, the effect of BNCT on normal bonein mice were evaluated regarding to their bonestrengths. The tibial bending strength was decreased by reactor-producing radiation including thermal neutron, epithermal neutron, fast neutron, and γray. However, the effect of BPA administration onbone strength was expected to be minimal.

35

7KHHIIHFWRIERURQQHXWURQFDSWXUHWKHUDS\ %1&7 RQQRUPDOOXQJLQPLFH
month.

M. SuzukiDQG Y. Tamari

IQVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 An accelerator-based boron neutron
capture therapy (BNCT) system and boronophenylalanine(BPA)-based new drug were approved by the Ministry of
Health, Labour and Welfare of Japan for the treatment oflocally unresectable recurrent or unresectable advanced
head and neck cancer on March 2020. Since BNCT will
be carried out at the medical institute, the accessibility of
BNCT will improve dramatically and much greater patients will be treated with accelerator-BNCT comparedwith reactor-BNCT. One of the drawbacks of BNCT isthat thermal neutrons necessary for tumor control cannot
be delivered to the deep portion of the tumor which is located at > 6 cm in depth from the skin surface.
For BNCT to be recognized as effective treatment modality for malignant tumors, to expand indication of
BNCT is very important. We have investigated the possibility of BNCT for malignant tumors in body trunk suchas liver and lung cancers. In these body trunk tumors,
multiple lung metastatic tumor is good candidate for new
application. Since the lung contains air, thermal neutron
is delivered to the lung tissues in deep portion. In BNCT
for multiple lung tumors, whole lung is irradiated with boron thermal neutron capture irradiation.
We have investigated the compound biological effectiveness (CBE) factor for normal lung tissues. The CBEfactors depend on the biological or clinical endpoint.
The CBE factor for normal lung tissue had been reported
at 2.3 from the Massachusetts Institute of Technology(MIT) group. In MIT study, the biological endpoint for
the CBE factor was the occurrence of lung fibrosis. In
our study, the clinical endpoint for the CBE was the death.
We have already reported the survival fraction following whole thorax irradiation with X-ray irradiation. In
2020, the effect of thermal neutron beam at KUR on normal lung was investigated.
(;3(5,0(176 Ten to twelve-week old female
C3H/He mice were used. Since, in this experiment, alarge amount of thermal neutrons were needed to cause
equivalent biological effect with X-ray irradiation, the irradiations were carried out at the 5MW reactor power.
The mice were anesthetized by intraperitonial injection ofpentobarbital solution (5 mg/ml in saline) at the dose of 10
Pl/g. The three or four mice were fixed in the paper box
and the body except for the thorax were shielded with LiF
plate. The mice were sorted into four treatment groups,
40-min, 50-min, 60 min, and 70-min irradiation groups.Ineach group, six to seven mice were treated. The acrylbox containing mice were irradiated with thermal neutron
beam at the thermal neutron flux of 7.5E+09 n/cm2/s
which was measured by analysis of activation of gold foil
attached to the surface of the box. Survival and change
of weight have been observed twice or three times a week
in the first one month and once a week after the second

31P10-1‑93‑

5(68/76 In 40-min and 50-min irradiation groups, all
the mice survive within an observation period of 40 to 140
days. In 60-min irradiation group, six mice died within
an observation period of 12 days, three mice survive
within an observation period of 140 to 180 days, and one
mouse died at 146 days after the treatment. In 70-min irradiation group, all the three mice died within 10 days.
Figures.1-3 show the weight change of the 40-min, 50-min,and 60-min treatment groups. In all the groups, 20 to 40%
weight reduction was observed within two weeks.

',6&866,21 In X-ray irradiation group, the micetreated with 16-17 Gy died within an observation period of
120 to 300 days. The survival of mice irradiated withthermal neutron beam will be compared with that of micetreated with X-ray irradiation in 2020.

35

6WXG\RIWKHLQIOXHQFHRQQRUPDOOLYHUWLVVXHE\%1&7

Y. Tamari1, S. Takeno, T. Takata, M. Suzuki

showed a tendency for increased liver fibrosis in the neutron-irradiated group receiving BPA (BNCT group). The
result of HE staining demonstrated that the steatosis of
the BNCT group was increased. Furthermore, quantification of triglyceride was performed to determine the degree of steatosis of normal mouse liver tissue after BNCT.
Triglycerides in mouse normal liver tissue after BNCT
tended to be increased compared to control. Furthermore,as a result of Western blotting, the expression of sonichedgehog protein in the BNCT group was higher than in
the group only irradiated with neutrons.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
'HSDUWPHQWRI5DGLRORJ\.\RWR3UHIHFWXUDO8QLYHUVLW\RI0HGLFLQH
,1752'8&7,21  Boron neutron capture therapy(BNCT) for liver tumor, which has been conducted up to
the present, has used the compound effectiveness factor(CBE) determined by using genotoxicity for hepatocytes
as an indicator, which has been clarified by Suzuki et al[1]. But there is a problem whether it is appropriate as areal clinical endpoint. Fundamental researches of liver
fibrosis that are the late effect of radiation therapy arenecessary. It is necessary to do basic research that uses
liver fibrosis, which is a late radiation injury to the liver,as an evaluation index. The hedgehog signaling pathway
is one of the important processes involved in animal development, and has been implicated in the maintenanceand regeneration of adult tissues. The hedgehog signaling
pathway is activated in the damaged liver and affects
tissue remodeling. It has also been reported that cell proliferation is promoted and epithelial-mesenchymal transition leading to fibrosis is induced [2][3]. A purpose ofthis study is to establish systematically and continuously
technique that can analyze the harmful phenomenon in
the normal liver tissue of BNCT.
(;3(5,0(176 Female C57BL6 mice at 6weeks
of age were injected 1000mg/kg p-boronophenylalanine(BPA) solution Subcutaneously 2 hours before neutron
irradiation. The mice were irradiated for 60 minutes at
the 1MW output. One week after irradiation, mice weresacrificed and the blood and livers were analyzed. Blood
and liver boron concentrations 2 hours and 3 hours after
the administration of 1000 mg / kg BPA were quantified
using Inductively Coupled Plasma Spectrometer (ICP).
The livers of the mice 6 months after neutron irradiation
were stained with Masson trichrome. HE staining andtriglyceride quantification were performed to investigate
degree of the steatosis in the mouse normal liver tissue
after BNCT. Western blotting was performed to determine the expression level of Sonic Hedgehog protein. In
addition, Masson trichrome staining was performed todetermine the degree of liver fibrosis six months after
neutron irradiation.

Fig.1 Triglyceride concentration of mouse liver. A significant difference was observed comparing the control and
BNCT groups. (**). Error bars indicate standard deviationsFig.2 Shh expression level after neutron irradiation. Upper bar is Shh and Under bar is GAPDH of Ctrl (Control)and Nut (Neutron alone), 1000 (BNCT group).
5()(5(1&(6>@ M. Suzuki HWDO, Jpn. j. Cancer. Res., (2000)
1058-1064.
>@ Y. jung et al., Gut, 59 (2010) 655-665.
>@ F. Rangwala HWDO, J. Pathol., 224 (2011) 401-410

5(68/76 Two hours after the administration of BPA,
the liver boron concentration was about 8.1 μg/g, and theblood boron concentration was about 9.2 μg/g. Threehours after BPA administration, the liver boron concentration was about 4.1 μg/g, and the blood boron concentration was about 4.4 μg/g. Masson trichrome staining

P10-4‑94‑35

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‑96‑

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M. Suzuki,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH .\RWR
8QLYHUVLW\

The isotope of gadolinium-157 (157Gd) has the highest
thermal neutron capture cross-section about 254,000 barnwhich is about 66 times higher compared with that of boron-10 (10B). The gadolinium neutron capture reaction
is as follows, 157Gd+n = 158Gd+gannma-ray+internalconver-sion elections +Auger electrons.
Among thebyproducts, Auger electrons is categorized as a highlinear energy transfer radiation which can induce double
strand brake of DNA. Since the range of the Auger
electron is the order of a few nanometers, cell killing
effect by the electron is evoked at when 157Gd isincorporated into the target such as DNA. Combination
therapy with BNCT and Gd-NCT may help to raise theradiation dose for the deep portion of the tumors.

HIIHFW ZRXOG EH DVFULEHG IURP D KLJKHU *GUHWHQWLRQLQ
WKHWXPRUWLVVXHDQGLPSURYHGGLVWULEXWLRQRI *G ZLWKLQWUDWXPRUDOO\ DGPLQLVWHUHG *GQDQR&3
3 Tetra (methylene phosphonic acid) chelate of Gd(Gd-EDTMP) were evaluated with reference to tissue distribution and effects of thermal neutron irradiation using
tumor animal models. Malignant melanoma B16 cells administered through the caudal artery infiltrated the bonemarrow in all of the mice. In addition, 157Gd was distributed in the bone matrix around the bony edge line andmalignant melanoma. When the distribution of malignant
melanoma was compared according to the distribution ofmelanin in the thermal neutron irradiated andnon-thermal neutron irradiated groups, no significant
difference was found in the present study.

3 In this study, to construct the molecular system
to take drugs into cell nucleus was attempted by using
Hoechst molecules. Since the Hoechst group
has high DNA-binding function and accumulates in
the cell nu- cleus, it was expected that this molecule act
as a courier molecule to deliver drugs into the nucleus.
Herein, we designed the reaction protocols to couple
the drugs with Hoechst unit by Huisgen cycloaddition
reaction.
3 The results showed that the chicken egg CAM
model can be used as a model to examine the efficacyof the GNCT therapy. The results of gadoliniumloaded nanoparticles compared with that of free gadolinium compound show that the nanoparticle formulation increases efficacy of GNCT.
3In this study, a series of nanocarriers in sub-50
nm scale and researched its antitumor effect though thechange of tumor size was investigated as a novel Gdcompound. The growth rate of the C26 tumors was
significantly inhibited after injection of PEG272 andPEG454 with irradiation compared with non-irradiationgroup.
3In this study, a silica nano-particle (SiNP, 61.6
ʸ 3.8 nm in diameter) containing 55 ng/mg
Gd3TCAS2, which is promising as a carrier for GdNCTwas investigated as a new Gd-compound.

In this research project, eight research projects were
included. Details of each project is referred to thefollowing contents.
3 In the case of irradiation to the cell incorporating
157

Gd compound which are suspended liquid, the cells areirradiated with gamma-ray (range is >100 Pm) which are
emitted from surrounding the cells. To eliminate the irradiation by gamma-ray as much as possible, the irradiation
system as follows is effective; the cells adhered to the wellof the microplate which stands upright are irradiated withthermal neutrons. A preliminary experiment study was carried out to confirm the feasibility of the irradiation system.
Since the point to notice is occurrence of contamination,
the microplate should be sealed by sterilized seat to keep
the medium in the well of microplate. During the observation time for one week, no contamination was experienced. With respect to the cell killing effect, the BPAtreated cells were morphologically destructed and decreased in number compared with no treatment and irradiation alone control groups.
3In this study, the effectiveness of new Gd-loaded
nanoparticle was tested in vivo study. Since this study was
carried out as preliminary study, only one mouse was used.
The GdXX-NCT showed a little growth inhibition compared with that of thermal neutron irradiation.
3 ,Q WKLV VWXG\ ZH LQYHVWLJDWH WKH LQ YLYRDQWLWXPRUHIIHFWVDIWHU1&7ZLWKLQWUDWXPRUDOLQMHFWHGQDQRSDUWLFXODWH IRUPXODWLRQV *GQDQR&3V ZLWKGLIIHUHQWSDUWLFOHVL]HVZHUHSUHSDUHGE\XVLQJFKLWRVDQZLWK PROHFXODU ZHLJKWV RI  N *GQDQR&3   RU
 N *GQDQR&3   DQG *G'73$ WKURXJK WKHSUHYLRXVO\ GHYHORSHG ZR HPXOVLRQGURSOHW FRDOHVFHQFH WHFKQLTXH  7KH *GQDQR&3  H[KLELWHG D
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7KLVVLJQLILFDQFHLQWXPRUNLOOLQJ

3

‑97‑

35

,QYHVWLJDWLRQRIFHOONLOOLQJHIIHFWE\DXJHUHOHFWURQVHPLWWHGGXULQJJDGROLQLXPQHXWURQFDSWXUHWKHUDS\ *G1&7 

M. SuzukiDQG H. Tanaka

IQVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 An accelerator-based boron neutron
capture therapy (BNCT) system and boronophenylalanine(BPA)-based new drug were approved by the Ministry of
Health, Labour and Welfare of Japan for the treatment oflocally unresectable recurrent or unresectable advanced
head and neck cancer on March 2020. Since BNCT will
be carried out at the medical institute, the accessibility of
BNCT will improve dramatically.
One of the drawbacks of BNCT is that thermal
neutrons necessary for tumor control cannot be delivered
to the deep portion of the tumor which is located at > 6
cm in depth from the skin surface. To overcome thedrawback, in the clinical study on BNCT for malignant
glioma, X-ray irra-diation to the deep portion of thetumor was followed by BNCT.
The isotope of gadolinium-157 (157Gd) has the highest
thermal neutron capture cross-section about 254,000 barnwhich is about 66 times higher compared with that of boron-10 (10B). The gadolinium neutron capture reaction
is as follows, 157Gd+n = 158Gd+gannma-ray+internalconver-sion elections +Auger electrons.
Among thebyproducts, Auger electrons is categorized as a highlinear energy transfer radiation which can induce double
strand brake of DNA. Since the range of the Auger
electron is the order of a few nanometers, cell killing
effect by the electron is evoked at when 157Gd isincorporated into the target such as DNA. Combination
therapy with BNCT and Gd-NCT may help to raise theradiation dose for the deep portion of the tumors.
To investigate the cell killing effect by Auger electron,
irradiation by other byproducts yielded by 157Gd neutron
capture reaction should be eliminated as much as possible
from the site of the reaction. In the case of irradiation to
the cell incorporating 157Gd compound which are suspended liquid, the cells are irradiated with gamma-ray(range is >100 Pm) which are emitted from surroundingthe cells. To eliminate the irradiation by gamma-ray asmuch as possible, the irradiation system as follows is effective; the cells adhered to the well of the microplate
which stands upright are irradiated with thermal neutrons.
A preliminary experiment study was carried out to confirm the feasibility of the irradiation system. Since thepoint to notice is occurrence of contamination, the microplate should be sealed by sterilized seat to keep the medium in the well of microplate.
(;3(5,0(176 The colon-26 cells were maintainedin RPMI-1640 supplemented with L-glutamine and 10%
fetal bovine serum (FBS). The 1,000 cells per well wereseeded in the 96-well microplates. After overnight incubation, the medium of each well was replaced by BPAcontaining medium at the 10B concentration of 100 ppm
for 2 hours before irradiation with thermal neutron. The

31P11-1‑98‑

microplate was sealed with sterilized seat and kept standing upright. The microplate was irradiated with thermal
neutron beam at the flux of 1x109 n/cm2/s-1 for 30 minutes.
After the irradiation, the medium in each well was replaced with fresh medium. To confirm the feasibility ofthis experiment, the microplate was kept in the incubatorfor one week. The occurrence of contamination was visually checked and the cell killing effect by BPA-treated cells
was inspected thorough a microscope.
5(68/76 During the observation time for one week,
no contamination was experienced. With respect to thecell killing effect, the BPA-treated cells were morphologically destructed and decreased in number compared withno treatment and irradiation alone control groups.
',6&866,21  To irradiate the cells attached to the culture device vertically against the thermal neutron beam,
the irradiation system in which microplate was standing
upright was used in this experiment. Although some additional procedure such as sealing the plate with sterilized
seat is needed, the analysis of the cell-toxic effects such as
WST-1 assay is easily carried out by using microplate
reader. Since the feasibility of this irradiation system
was confirmed, we will investigate the cell killing effectof the positive-charged 157Gd-compound which was
at-tached to the cell membrane.

35

,QYHVWLJDWLRQRIJDGROLQLXPQHXWURQFDSWXUHWKHUDS\ *G1&7 
XVLQJJDGROLQLXPORDGHGQDQRSDUWLFOH

M. Suzuki, Li. Peng1, N. Komatsu1, Li. Zhao2

and the weight of the mouse was measured twice a week.
The tumor volume was calculated by the following equation:
The tumor volume = (long diameter x short diameter x
short diameter) / 2.
Since this preliminary experiment was carried out in accompanied with other experiment using 50-60 mice, thetumor growth curve for GdXX was compared with thoseof no-treatment control and thermal neutron irradiation
control in the other experiment.

IQVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI+XPDQDQG(QYLURQPHQWDO6WXG
LHV.\RWR8QLYHUVLW\
Medical College, Soochow University,1752'8&7,21An accelerator-based boron neutron
capture therapy (BNCT) system and boronophenylalanine(BPA)-based new drug were approved by the Ministry of
Health, Labour and Welfare of Japan for the treatment oflocally unresectable recurrent or unresectable advanced
head and neck cancer on March 2020. Since BNCT will
be carried out at the medical institute, the accessibility of
BNCT will improve dramatically.
One of the drawbacks of BNCT is that thermal neutronsnecessary for tumor control cannot be delivered to the deep
portion of the tumor which is located at > 6 cm in depth
from the skin surface. To overcome the drawback, in theclinical study on BNCT for malignant glioma, X-ray irradiation to the deep portion of the tumor was followed by
BNCT.
The isotope of gadolinium-157 (157Gd) has the highest
thermal neutron capture cross-section about 254,000 barnwhich is about 66 times higher compared with that of boron-10 (10B). The gadolinium neutron capture reaction is
as follows, 157Gd+n = 158Gd+gannma-ray+internal conversion elections +Auger electrons. Among the byproducts,
Auger electrons is categorized as a high linear energy
transfer radiation which can induce double strand brake ofDNA. Since the range of the Auger electron is the order ofa few nanometers, cell killing effect by the electron isevoked at when 157Gd is incorporated into the target such
as DNA. Combination therapy with BNCT and Gd-NCT
may help to raise the radiation dose for the deep portion of
the tumors.
In this study, the effectiveness of new Gd-loaded nanoparticle was tested in vivo study. Since this study was carried out as preliminary study, only one mouse was used.

5(68/76 Decrease of the weight of the GdXX-NCT
treated mouse 10% greater than that of the treatment day
was not observed. Fig.1 shows the tumor growth curves
for no-treatment control, thermal neutron irradiation, andGdXX -NCT treated mice. The GdXX-NCT showed alittle growth inhibition compared with that of thermal neutron irradiation.

',6&866,21No suggestion was drawn fromthis preliminary experiment in which only one mouse was treatedwith GdXX-NCT. In 2020, the pharmacokinetic and
GdXX-NCT in vivo studies were planned.

(;3(5,0(176 The colon-26 cells were maintainedin RPMI-1640 supplemented with L-glutamine and 10%
fetal bovine serum (FBS) in cell culture flasks (T-75).
The cells were processed into single cells by exposure of
0.05% trypsin. The single cell suspended medium was
prepared at the concentration of four million cells per 100
Pm. At 10 days before the irradiation, four million colon-26 cells in 100 Pm FBS-free medium were implanted
to the left hind leg of 8-week old female Balb/c mice. At
the irradiation, size of the tumors ranged from 10 cm to 15
cm. The new Gd-loaded nanoparticle (GdXX) was injected to one mouse intravenously via tail vain at 24 hours
before the irradiation. The mouse was irradiated at theheavy water facility of Kyoto University Research Reactor(KUR) at the thermal neutron flux of 5.1E10+8 (n/cm2/s)
for 60 minutes. The long and short diameter of the tumor

31P11-2‑99‑

35

Nanoparticulate formulations for neutron capture therapy:
Evaluation of anti-tumor effect after intratumor injection

T. Andoh1, T. Fujimoto2, M. Suzuki3, T. Takata4, Y. Sakurai4 and H. Ichikawa1
1

Faculty of Pharmaceutical Sciences, Kobe Gakuin University, Japan.
2
Department of Orthopaedic Surgery, Hyogo Cancer
Center, Japan.
3
Particle Radiation Oncology Research Center, Institutefor Integrated Radiation and Nuclear Science, Kyoto
University, Japan.
4
Division of Radiation Life Science, Institute for Integrated Radiation and Nuclear Science, Kyoto University,
Japan
INTRODUCTION: The successful treatment of cancer by neutron capture therapy (NCT) requires selective
delivery of large amounts of 10B or 157Gd isotope to tumor cells. In the previous study, we developed two types
nanoparticulate formulations for NCT. One is formulated
nanosuspension(NS)composedof
p-borono-L-phenylalanine (L-BPA) itself. In thisBPA-NS formulation, solid particles of L-BPA are dispersed in water with a surface-active stabilizer. The otherone is gadolinium-loaded chitosan nanoparticles(Gd-nanoCPs). Gd in Gd-nanoCP-treated tumors is based
primarily on the bioadhesive (cationic), biocompatible(nontoxic), and biodegradable (bioerodible) properties ofchitosan nanoparticles. In the present study, we investigate the in vivo antitumor effects after NCT with intratumoral injected nanoparticulate formulations.
EXPERIMENTS:
Macrogol 15 hydroxystearate(Solutol® HS 15, SO) and soybean lecithin (SL) wereused as stabilizers. BPA-NS using SO and SL was prepared by a wet-milling method with the use of a Pulverisette-7 planetary ball mill (Fritsch). The obtained
BPA-NS was sonicated using a 2510J-DTH water-bathsonicator (Branson Ultrasonics Co.) for 5 min at room
temperature. Gd-nanoCPs with different particle sizes
were prepared by using chitosan with molecular weightsof 10 k (Gd-nanoCP 200) or 950 k (Gd-nanoCP 400) andGd-DTPA through the previously developed w/o emulsion-droplet coalescence technique [1]. In the NCT trial,
male B16F10 melanoma bearing C57BL/6J mice wereused. The mice were divided into NCT group and HOT
control group. BPA-Fructose complex (BPA-Fr), BPA-NS(500 mg BPA/kg), Gd-nanoCP 200 and 400 (2.4 mg
Gd/kg) were administered intratumoral (i.t.) injection to
the mice. The tumors in the left hind legs were exposedto thermal neutron irradiation at the Institute for Integrated Radiation and Nuclear Science, Kyoto University.
For determining the tumor volume, two bisecting diame-ters of the tumor were measured with a slide caliper, andcalculation with the longest and shortest length of thetumor in millimeters (mm). The tumor-growth suppressing effect was assessed by the ratio of tumor volume before and after neutron irradiation.
RESULTS: BPA-NS displayed a mass median diameter of 176 nm. After i.t. administration, BPA-NS gave riseto the remarkably prolonged retention of 10B in tumor
tissue possibly due to the slow diffusion and/or dissolution of solid BPA-nanoparticles in a tumor. Gd-nanoCPs
prepared using chitosan with a higher MW (950 kDa) had
a mean particle size of 468 nm; Gd-nanoCPs preparedusing chitosan with a lower MW (10 kDa) had a mean
particle size of 185 nm. After i.t. administration,
Gd-nanoCP 200 showed significantly higher Gd concentration in tumor tissue in comparison to Gd-nanoCP 400.
In the NCT trial, growth of tumor masses was observedin the control group, while the NCT groups showed anequivalent suppression of tumor growth (Fig. 1). In
BNCT, two BPA formulations had been similar tumor-killing effect. These results suggested that boron
accumulates specifically in the tumor after i.t. administration of BPA formulations and that BNCT after i.t.
dosing of BPA-NS is equally efficacious in the treatmentof BNCT after i.t. administration of BPA-Fr. In GdNCT,
the Gd-nanoCP 200 exhibited a stronger tumor-killing
effect than the Gd-nanoCP 400. This significance in tumor-killing effect would be ascribed from a higher Gdretention in the tumor tissue and improved distribution of
Gd with intratumorally administered Gd-nanoCP 200.

Fig. 1. Tumor volumes after thermal neutron beamirradiation of NCT and HOT control groups.
REFERENCES:[1] H. Tokumitsu et al., Pharm. Res., 16, 1830–1835(1999).

31P11-3‑100‑

35([DPLQDWLRQ RQ JDGROLQLXP QHXWURQ FDSWXUH WKHUDS\ LQ PRXVHPDOLJQDQW PHODQRPD ERQHPHWDVWDVLVPRGHO

T. Matsukawa1, A. Kubota1, M. Suzuki2, A. Shinohara1,3,
K. Kajino1, K. Yokoyama1,4

-XQWHQGR8QLYHUVLW\)DFXOW\RI0HGLFLQH,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
5HVHDUFK,QVWLWXWHIRU&XOWXUDO6WXGLHV6HLVHQ8QLYHUVLW\,QWHUQDWLRQDO8QLYHUVLW\RI+HDOWKDQG:HOIDUH
,1752'8&7,21 To develop the next generation ofcancer radiotherapy, we evaluated tissue distribution andeffects of thermal neutron irradiation on tumor animalmodels of tetra (methylene phosphonic acid) chelate of
Gd (Gd-EDTMP), a neutron capture therapy formulation
containing gadolinium. The distribution of 157Gd in thetissue was imaged by laser ablation inductively coupledplasma mass spectrometry (LA-ICP-MS).
(;3(5,0(176 Gd-EDTMP solutions were prepared from gadolinium chloride and EDTMP;
C57BL/6JJcl female mice (6 weeks old) were obtained
from CLEA Japan, Inc. (Tokyo, Japan). Mouse malignant
melanoma B16 cells (JCRB0202) were purchased fromJCRB Cell Bank (Ibaraki, Japan). Cultured B16 cells
were injected from the tail artery of C57BL mice anesthetized with isoflurane and transplanted into the lower
limbs (1×106 cells per mouse). On day 7 after transplantation, a saline dilution solution of Gd-EDTMP was administered intraperitoneally at a concentration of 20.0
mg-Gd/kg. After 24 h of injection, mice were randomly
divided into two groups (n = 3) and one group was irradiated with thermal neutrons at the Kyoto University reactor at 6.0 × 108 cm-2 for 60 min. The remaining one group
was not irradiated. After 7 days, mice were sacrificed andfemur and tibia were sampled. For each mouse, the left
femur was demineralized for 24 h, paraffin-embedded,
and 5 μm sections were made in thin sections parallel tothe long axis of the bone and stained with hematoxylin
and eosin (H.E.). The right femur was cut into thin sections every 5 μm using the Kawamoto method, anon-demineralized frozen section preparation method,
and the 157Gd distribution was determined by
LA-ICP-MS[1]. The invasion of the tumor into the bone
was assessed by micrographs of H.E. stained sections of
the femur and tibia.
5(68/76 Malignant melanoma B16 cells administeredthrough the caudal artery infiltrated the bone marrow inall of the mice studied here. In addition, 157Gd was distributed in the bone matrix around the bony edge line andmalignant melanoma. When the distribution of malignant
melanoma was compared according to the distribution ofmelanin in the thermal neutron irradiated andnon-thermal neutron irradiated groups, no significant
difference was found in the present study.
Although bone is hard tissue, it is actually undergoing

constant remodeling by osteoblasts and osteoclasts.
Gd-EDTMP may have been included in this remodeling.
In bone metastatic tumors, tumor cells that flow into thebloodstream create a foothold in the bone marrow, disrupting the balance between osteoclasts and osteoblasts
and proliferating. It is known that there are many cases ofosteoclastic enhancement due to tumor growth, and it isthought that 157Gd is enriched by the incorporation of
Gd-EDTMP into the bone tissue generated by osteoblasts
that work for repair in the vicinity of these osteoclasts. In
particular, the acidic environment caused by osteolysis is
known to be one of the causes of pain, so this formulation,
which can capture neutrons in the vicinity, may have aneffect on the pain of bone metastases. In the present study,
there was no significant difference in the distribution ofmelanin in malignant melanoma caused by thermal neutron irradiation, which may be due to the small number ofanimal models produced and the fact that we could notcompare the malignant melanoma cells themselves because we used pigment as an indicator. In the future, it isnecessary to study the experimental animal model systemthat can follow the therapeutic effect of neutron capture
more strictly, especially the model focusing on the painof bone metastasis.

宆室季

孷孶

孴學孺

宊宧季

Fig. 1.
Distribution of 43Ca and 157Gd in the tumor bearing mice femur 24h after injection of Gd-EDTMP.

5()(5(1&(6[1] A. Kubota HW DO, Juntendo Medical Journal., (2019) 461-467.

31P11-4‑101‑

35

3UHSDUDWLRQRIGUXJVEHDULQJ+RHFKVWXQLWWKDWWDUJHWFHOOQXFOHXV

K. Tanabe, M. Suzuki, T. Nishihara and J. Meguro'HSDUWPHQWRI&KHPLVWU\DQG%LRORJLFDO6FLHQFH&RO
OHJHRI6FLHQFHDQG(QJLQHHULQJ$R\DPD*DNXLQ8QL
YHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 The cell nucleus has been recognized as an important target in boron neutron capture
therapy (BNCT). Therefore, there are increasing demands
for the development of the methods to take drugs for
BNCT to cell nucleus.
In this study, we attempted to construct the molecularsystem to take drugs into cell nucleus by using Hoechst
molecules. Since the Hoechst group has high DNA−binding function and accumulates in the cell nu-cleus,1,2
it was expected that this molecule act as a courier
molecule to deliver drugs into the nucleus. Herein, we
designed the reaction protocols to couple the drugs with
Hoechst unit by Huisgen cycloaddition reaction.
(;3(5,0(176+XLVJHQ F\FORDGGLWLRQ UHDFWLRQ EHWZHHQ $+RHFKVW
DQG D]LGHPHWK\ODQWKUDFHQH  A-Hoechst (1.0 mg,
2.2 Pmol) was added to the solution of
9-azidemethylanthracene (0.5 mg, 2.1 Pmol) in
DMF-H2O. Then, CuSO4, TBTA and sodium ascorbate
were added to the solution. The resulting mixture wasstirred for 20 h at ambient temperature. After the reaction,
the mixture was extracted with ethyl acetate. The organic
layer was washed with brine, dried over MgSO4, filteredand concentrated in vacuo. The crude product was purified by silica gel column chromatography to give anthracene derivative with Hoechst unit 12.
5(68/76 We designed the synthetic protocols of the
Hoechst-tethered molecules by using Huisgen cycloaddition. It is well-known that azide group is coupled withacetylene unit in the presence of Cu(I) catalyst via a formation of triazole ring. Thus, we designed Hoechst unit
with acetylene group (A-Hoechst in Scheme 1) and drugs
with azide substituent.
The synthesis of A-Hoechst is outlined in Scheme 1.
Phenol derivative 1 was alkylated by propargyl bromide
under basic conditions to form 2. On the other hand, dinitro benzoic acid 3 was converted to amide 4, and then 4
was reduced to give diamine 5. The diamine 5 was treated with aldehyde 2 to form benzimidazole derivative 6,
which was reduced to give formyl benzimidazole 7. The
Hoechst skeleton was synthesized as follows. Nitroaniline 8 was coupled with 1-methylpiperazine under basic
conditions and following reduction gave diaminobenzene
10. The coupling of 7 and 10 furnished the desired
A-Hoechst.
We next evaluated the Huisgen reaction of A-Hoechst. Asa phantom drug, we employed 9-azidemethylanthracene
11 and conducted the cycloaddition reaction. The reactionof A-Hoechst and anthracene 11 was conducted at ambient temperature in the presence of catalytic CuSO4 andascorbic acid. Efficiently, the triazole ring formation occurred, and anthracene derivative with Hoechst unit 12
was formed. These results strongly indicate that
A-Hoechst will be a promising molecule to prepare
Hoechst-tethered molecules. At present, introduction ofGadolinium complexes or boron compounds into
A-Hoechst is in progress.

6FKHPH  Reagents and conditions (a) Propargyl bromide, K2CO3, DMF, 80 qC, 3 h, 71% (b) SOCl2, 80 qC,
1.5 h; N,O-Dimethyldroxylamine Hydrochloride, pyridine, CH2Cl2, r.t, 3.5 h, 63% (2 steps) (c) H2, Pd/C, EtOH,
r.t, 3 h (d) 2, Na2S2O5, H2O, 90 qC, 5.5 h, 64% (2 steps)(e) LiAlH4, THF, 0 qC, 1 h, 74% (f) 1-Methylpiperazine,
K2CO3, DMF, 90 qC, 3.5 h, 55% (g) H2, Pd/C, EtOH, 90
qC, 5 h (h) 7, Na2S2O5, H2O, 90 qC, 1 h, 80%.

)LJXUHHuisgen reaction between A-Hoechst and 11.5()(5(1&(6>@ Tsukiji, S. et al., &KHP&RPP (2014) 6149–6152
>@ Tanabe, K. et al., &KHP%LR&KHP, (2018) 956-962.

31P11-5‑102‑

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K. Matsumoto, A. Komatsu, Y. Higashi, M. Tamari, M.
Suzuki and F. Tamanoi

5(68/76
Exp.1:
Three days after transplanting human ovarian cancer cells
onto the CAM membrane, tumor formation was confirmed. The tumor was examined by green fluorescenceof ovarian cancer cells that express GFP. In addition,
H&E staining of the tumor was carried out.

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Gadolinium Neutron Capture Therapy (GNCT) provides
a promising alternative to BNCT. Because gadolinium isused as an MRI enhancing reagent, various compounds
containing gadolinium have been developed. Our aim isto establish a capability to test various gadolinium containing reagents for GNCT at the Kyoto University Research Nuclear Reactor. In this study, we have evaluatedthe possibility to use the chicken egg tumor model thathas been shown to be effective for the study of BNCT.
Nanoparticles can be tuned to accumulate in the tumor.
This feature is attractive for GNCT, as tumor accumulation of gadolinium may dramatically enhance GNCT efficacy. We chose mesoporous silica-based nanoparticles
as a carrier for gadolinium. This material is a homogeneous preparation of nanoparticles with a diameter of
40-400 nm. Approximately 1400 pores are present in one
particle. Because the wall of the pore can be considered
as a part of the surface area, they have a large surface
area; it is reported that 1g of the nanoparticle contains
400 square meter of surface area.
(;3(5,0(176(Exp.1) The CAM assay was established by using fertilized chicken eggs. After incubation for ten days, a window was made on the egg shell and ovarian cancer cells
were transplanted onto the CAM membrane of fertilized
chicken eggs. Tumor formation was examined.

Exp.2:
Successful synthesis of gadolinium-loaded silica-based
nanoparticles was confirmed by SEM, TEM and elemental mapping using TEM (EDX-TEM). The size of thenanoparticle was 120 nm. Loading of gadolinium was 4%of the weight of the nanoparticle, as determined by ICP.
Exp.3:
We carried out a GNCT experiment using the nuclear
reactor. Gadolinium-loaded nanoparticles were intravenously injected into the chicken egg and irradiated with aneutron beam for one hour two days after the injection.
Three days after the irradiation, the size and weight of thetumor was examined. The results showed that the weightof the tumor after injection of gadolinium-loaded nanoparticles was 27% of the control tumor (no injection).
This contrasts with the injection of free gadolinium
compound in which case the weight of the tumor was
75% of the control. Nanoparticles without gadolinium
gave results that were similar to that of the control&21&/86,21$1')8785(35263(&76
Our results show that the chicken egg CAM model can beused as a model to examine the efficacy of the GNCT
therapy. The results of gadolinium-loaded nanoparticles
compared with that of free gadolinium compound showthat the nanoparticle formulation increases efficacy of
GNCT. However, this should be taken as a preliminary
result, as the experiment was carried out only once. Further experiments are planned using different conditions
such as varying irradiation time.

(Exp.2) Mesoporous silica-based nanoparticles weresynthesized by incubating TEOS in an alkaline solution
which promotes the formation of the Si-O-Si framework
as a base structure of the nanoparticle. CTAB was added
as a templating agent. Surface modification was carriedout by the grafting method that enabled attachment ofgadolinium to the surface of the nanoparticles. Stabilityof the gadolinium attachment was examined.
(Exp.3) The CAM model established as described in Exp.
1 was used to intravenously inject gadolinium-loaded
nanoparticles and the eggs were exposed to neutron at thenuclear reactor for 1 hour. Effect on tumor growth was
examined by observing tumor size as well as by examining tumor weight three days after the exposure.

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< 6DNXUDL.0RXUL<8HGD1'HZL
H. Cabral2, Y. Morishita7, T. Kanai8, S. Dowaki8,
T. Nagasaki8, Y. Sakura9, H. Tanaka9, M. Suzuki9,
S. Masunaga9, and H. Takahashi1,2,3

same samples but without receiving irradiation as controls groups. Besides, while measuring the size of tumor,
the weight change was also recorded for evaluation of the
toxicity of these samples.

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

INTRODUCTION:
Gadolinium neutron capture therapy (GdNCT) isa promising cancer treatment. Compared with theconven-tional boron NCT, because Gd compound canbe used as MRI contrast agent [1], it allowed for
MRI-guided GdNCT. However, clinical Gd-chelates
lack high and selective accumulation in tumors forelecting safe and potent GdNCT [2].
Nanoscale drug carriers are a promising way to
pro-mote the accumulation of Gd agents in tumors
through the enhanced permeability and retention(EPR) effect, which is based on the leaky vasculatureof tumor tissues and their impaired lymphaticdrainage. For developing successful nanocarriers for
GdNCT, it is necessary to design systems with high
Gd loading capacity that avoid leakage of free Gd.
Thus, we developed a series of nanocarriers in
sub-50 nm scale and researched its anti-tumor effectthough the change of tumor size.
EXPERIMENTS:
We developed nanocarriers based on poly(aspartic
ac-id) (P(Asp)) and were modified with poly(ethylene
gly-col) (PEG) chains having different molecularweight (Mw). After chelating Gd-DOTA, the final
products, whichare
PEG272(PEG272-P(AspGd-DOTA))
andPEG454(PEG454-P(Asp-GdDOTA)), were made.
Colon 26 cancer cell was used for the LQ YLYR
an-ti-tumor effect evaluation. After 24h administration,
the tumor-bearing mice received neutron irradiation
60 minutes at Nuclear Reactor Facility of Kyoto Univ
Insti-tute for Integrated Radiation & Nuclear Science
with average neutron fluence of 2.0 × 1012 n/cm2. thechange in tumor growth and survival rate of the micereflected the anti-tumor effect of nanocarriers.
Considering the influence of irradiation, we also set
the mice injected

5(68/76
The result of tumor growth showed at Figure 1. From
the results of antitumor effect after GdNCT (Fig. 1), thegrowth rate of the C26 tumors was significantly inhibited
after injection of PEG272 and PEG454 with irradiationcompared with non-irradiation group. However, PEG272
showed more potent antitumor ability. From day 9, therelative tumor volume became smaller than before irradiation, and until day 24, the relative tumor volume was
0.27 of the initial size. Despite PEG454 showed higher
tumor accumulation, the enhancement of the antitumor
activity of PEG272 could be attributed to the higher cellular uptake, as intracellular delivery of Gd has been indicated to be critical for effective cell killing [3].

)LJ7XPRUJURZWKVXSSUHVVLRQUHVXOW
Moreover, the body weight of the mice did not decrease after the treatments, which indicate the safety ofthese polymers and the GdNCT (Fig. 2).

Fig2. The weight loss
REFERENCES:[1] A. Narmani HW DO. J. Drug Deliv. Sci. Technol.,  2018457466
>@ H. Tokumitsu HWDO. Pharm. Res.  1999 1830–1835
>@ K. H. Jung HW DO. Contrast Media Mol. Imaging. 01 3727109

31P11-7‑104‑35

Development of Nano Carriers Installed with Gd(III)-Thiacalixarene
Complex for Gd-NCT

T. Yamatoya1, T. Nagasaki2, N. Iki1 and M. Suzuki3those samples with irradiation of thermal neutron, suggesting that the experimental conditions such as irradiation time were too harsh for the cell. Optimization of theirradiation conditions is necessary for further survey ofthe potential of the Gd-carrier.

1

Graduate School of Environmental Studies, Tohoku
University
2
Graduate School of Engineering, Osaka City University
3
Institute for Integrated Radiation and Nuclear Science,
Kyoto University

INTRODUCTION: Owing to a large thermal neutron
capture cross section and total kinetic energy of157
Gd(n,J)158Gd larger than that of 10B(n,D)7Li, gadolinium attracts growing attention as an alternative to boronin neutron capture therapy [1]. Because free gadolinium(Gd(OH2)9) has toxicity, a safe carrier of Gd to tumor not
to release free Gd is required. We recently found thatthiacalix[4]arene-p-tetrasulfonate (TCAS) self-assembled
three lanthanide (Ln) cores including Gd to form a sandwich-type complex, Ln3TCAS2 (Fig. 1) [2], the characteristic features of which are high kinetic stability, luminescence signal [3], and 1H relaxation arising from the Lncenter [4]. Nano-sized particles are frequently used as adrug carrier toward tumor by enhanced permeability andretention (EPR) effect. Previously, we obtained a silica
nano-particle (SiNP, 61.6 r 3.8 nm in diameter) containing 55 ng/mg Gd3TCAS2, which is promising as a carrierfor Gd-NCT. Here we attempted to evaluate the ability tokill cancer cell upon neutron irradiation by comparison
with the cases of Gd3TCAS2, BSA-Gd3TCAS2 complex,
Gd-DTPA, and PBS control.
EXPERIMENTS: Preparation of SiNP installed with Ln.
The trinuclear complexes Ln3TCAS2 (Ln = Gd, Tb) wereprepared as reported elsewhere [2]. The Ln3TCAS2installed SiNP was prepared by a Stöber’s method [5],
which
was
modifiedwithusing
3aminopropyltrimethoxysilane (APTES) as an anchor ofnegatively charged Ln3TCAS2. Furthermore, the surface
was modified with poly(ethylene glycol) (PEG) by PEGNHS (MW 2000) to retain water-dispersibility andbiocompatibility.
Cell experiments. MCF-7 cells were seeded in a 6-wellplate at a cell concentration of 1.0 × 105 cells/mL andincubated for 24 h. After supernatant was removed,
DMEM and solution of SiNP loaded with Gd3TCAS2 (5.0
× 105 M as Gd) were added to each well and incubated for
24 hr. After washing with PBS, the cells were de- tachedfrom the well and transferred to tubes to be irradi- atedwith thermal neutron (8.6 × 1012 n/cm2) for 90 min. Assay:
To the wells containing 2 mL of RPMI medium in 6-wellplates, irradiated cells were seeded at the concen- tration of
1,000 cells/well. After incubation for 14 days, the colony
was stained with crystal violet.
RESULTS:
The images of 6-well plates for samples without irradiation showed formation of colonies (Fig. 2). This implies
that Gd3TCAS2, BSA-Gd3TCAS2, and Gd3TCAS2-loaded
SiNP are not toxic. By contrast, no colony was found forFig. 1 Structure of Ln3 TCAS2 complex.

Fig. 2 Images of plates for the colony assay of MCF-7
cells with and without irradiation of thermal neutron.
REFERENCES:[1] M. Takagaki et al., Future Application of Boron and
Gadolinium Neutron Capture Thrapy, in Boron Science,
Ed N. S. Hosmane (CRC Press) (2012) 243.
[2] N. Iki et al., Eur. J. Inorg. Chem., 2016 (2016) 50205027.
[3] R. Karashimada et al., Chem. Commun. 52 (2016)3139-3142.
[4] N. Iki et al., Inorg. Chem. 55 (2016) 4000-4005.
[5] W. Stöber et al., J. Colloid Interface Sci., 26, (1968)
62-69

31P11-8‑105‑

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A. Kinomura,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\
2%-(&7,9(6  Irradiation facilities of high-energy
particles for neutrons (Material Controlled irradiation
Facility), ions (e.g., Heavy ion irradiation facility) andelectrons (Temperature-controlled irradiation facilities,
KUR-LINAC) have been extensively developed at theInstitute for Integrated Radiation and Nuclear Science.
The developed facilities have been in operation andopened for joint research projects. One of the objectivesof this project is to further improve or optimize
irradiation facilities for advanced irradiation experiments.
As characterization techniques for irradiated materials,
a slow positron-beam system and a focused ion beamsystem have been developed and introduced, respectively,in addition to previous characterization facilities such as
an electron microscope, an electron-spin-resonancespectrometer, a bulk positron annihilation spectrometerand a thermal desorption spectrometer.
Another
objective is to introduce new techniques or reconsider
analytical methods of previously used characterization
techniques.
Based on these two objectives, we expect theenhancement of previous studies and the attraction of
new users for the joint research program.
The allotted research subject (ARS) and individual
co-researchers are listed below. Note that the titles ofresearch subjects are based on individual reports.
ARS-1:
Study to improve transport and measurement
performance of a slow positron beamline (A. Kinomura
et al.)
ARS-2:
Electron-irradiation induced defects in W-Re (K. Inoue etal.)ARS-3:
Change in the positron annihilation lifetime ofelectron-irradiated F82H by hydrogen charging (K. Satoet al.)
ARS-4:The effect of gamma-ray irradiation on luminescence
properties of collolidal Si nanocrystals (T. Nishimura etal.)
ARS-5:
Irradiation technique for study on corrosion resistance of
fusion divertor materials to liquid metal during irradiation(M. Akiyoshi et al.)
ARS-6:
Measurement of positron lifetimes of various
diamond-like carbon thin films (K. Kanda et al.)
ARS-7
Positron annihilation spectroscopy on diamond-likecarbon films (S. Nakao et al.)5(68/76 In ARS-1, transport and measurement

performance of the KUR slow positron system wasevaluated with a positron beam during the KUR
operation. The brightness enhancement system andpositron lifetime measurement system were confirmed tobe effective.
In ARS-2, electron-irradiation to introduce only asimple Frenkel pair to W or W-5%Re (in weight %) was
performed. The effect of Re addition on the defectformation is investigated by the positron annihilation
method. Positron lifetime spectra before and after
elecron-irradiation were well fitted with one component
both even after irradiation.
In ARS-3, the quantity of hydrogen atoms trapped atvacancy clusters in electron-irradiated F82H wasevaluated by positron annihilation spectroscopy. The
samples were soaked with liquid nitrogen within 5 minfrom the end of hydrogen charging.
Isochronalannealing for 0.5 h was conducted every 25 K from 123
to 298 K. Subsequently, isothermal annealing was also
conducted at room temperature (298 K).
In ARS-4, the effect of gamma-ray irradiation on
luminescence properties of colloidal Si nanocrystals wasinvestigated. The heavy dose irradiation of gamma-rayon the colloidal Si nanocrystals causes the decrease inphotoluminescence intensity. A Compton effect on the
Si core of nanocrystal is attributed to thephotoluminescence quenching.
In ARS-5, irradiation techniques for study on corrosion
resistance of fusion divertor materials to liquid metal
during irradiation have been developed. Aluminum rich
ferritic steel (Fe-18Cr-3.3Al-0.4Si) NTK04L in liquid Sn
and FeCrAl-ODS in liquid Pb-Li were irradiated by
KURNS-LINAC in 1st and 2nd experiments in this year.
The validity of the developed specimen holders andmeasurement circuits was examined.
In ARS-6, free volume in the 4 kinds of DLC films
was evaluated by the results of positron annihilation
spectroscopy (PAS) and nano-indentation hardness.
Positron lifetime decreases with increasing hardness. The
relative S parameter also shows a tendency similar to a
positron lifetime, but does not completely agree.
In ARS-7, several types of DLC and carbon films werealso examined by PAS measurement for as-grown andthermally-annealed films. The results suggest that thestructural changes, possibly caused by hydrogen
desorption, may depend on the source gases and the films
prepared by C2H2 should be less stable than those
prepared by C7H8.
6800$5< Several new developments on irradiation(electron-beam and gamma-rays) and analyticaltechniques (beam and bulk positron measurements) for
new materials have been continuously performed in theline of the objectives of this project. Such studies may
enhance developments of new materials in various
scientific fields.

31P12

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A. Kinomura, N. Oshima1, Y. Kuzuya and A. Yabuuchi,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\
1DWLRQDO,QVWLWXWHRI$GYDQFHG,QGXVWULDO6FLHQFHDQG
7HFKQRORJ\ $,67 ,1752'8&7,21  Positron annihilation spectroscopy
is an important analytical method to detect vacancy-type
defects and vacant spaces of materials. Energy-variablemono-energetic positron beams (slow positron beams) areessential to perform depth-dependent positron annihilation spectroscopy of surface layers such as ion-implanted
layers or thin films formed on substrates. Intense positron sources are necessary to obtain slow positron beams
applicable for practical use. Positron sources based onpair creation, in general, provide higher intensity thanradioisotope-based positron sources. A positron source
using pair-creation by gamma-rays from a nuclear reactor
have been developed by using Kyoto University research
Reactor (KUR) to obtain a slow positron beam for materials analysis. In the KUR slow positron beamline, thesource size (converter and moderator assembly) is approximately 30 mm in diameter. For typical sample
sizes of materials analysis (<10 mm), it is necessary to
reduce beam sizes efficiently while keeping beam intensity as high as possible. For this purpose, brightness
enhancement techniques have been developed for the
KUR slow positron beamline [1]. In addition, measurement systems for positron annihilation lifetime spectroscopy have been optimized in this study.
(;3(5,0(176 The brightness enhancement systemof the KUR slow positron beam system has been evaluated in terms of the spot size and the beam intensity. A
single-crystalline Ni thin film annealed in vacuum at 750ºC for 1h was used as a remoderator of the brightness
enhancement system. The Ni remoderator film wascleaned by thermally excited hydrogen atoms after installation in vacuum to remove contamination during
handling in air.
In addition to the detailed studies of last year, the performance of the brightness enhancement system was
re-evaluated.
In particular, transport of a brightness-enhanced beam to the downstream and efficiency of
remoderator thin films were investigated again after
careful treatments of the remoderator film and measurements of beam intensities.
5(68/76 The trajectories of the beam were optimized by adjusting voltages for the source components
and currents for transport coils by observing images ofphosphor screens on microchannel plates (MCP’s). In
particular, the excitation current of the focusing lens of
the brightness enhancement system was optimized byobserving the spot images on the MCP screen positioned
at the focal point of the lens. The spot sizes at individual MCP screens were evaluated using photographs of the
spot images taken by a digital single-lens reflex camera
with a CMOS CCD (charge coupled device) image sensor.

To avoid unnecessary data processing in the camera, a
RAW-mode (a raw-data mode without data processing)was selected for this experiment. Linearity of used devices such as the MCP, the phosphor screen and the CCD
was taken into account. Parameters of image acquisition were appropriately selected to keep the linearity of
the combination of these three devices.
Figure 1 shows the images of the beam spots before
and after the brightness enhancement. The distributionof the beam spot were different for horizontal and verticaldirections. Furthermore, the positron source near thereactor core has a circular shape but the images of Fig.
1(a) was uneven (not circular). We believe that theoriginal beam (i.e., circular beam) extracted from thesource was cut several times by the walls of vacuum
ducts during beam transportation. Regardless of theseresults, we evaluated spot size as a full-width at
half-maximum (FWHM) value for horizontal and verticaldirections.
Demagnification factors calculated from the spot image were close to 1/10. The efficiency of the remoderator in the case of an extraction energy of 6.5 keV wasmeasured to be ~4% by gamma-ray intensities measured
from the MCPs placed before and after the brightness
enhancement system. As the beam loss at the acceleration mesh before the brightness enhancement was assumed to be 80%, the actual remoderation efficiency of
the Ni film was estimated to be higher than the measured
efficiency. The estimated efficiency value is acceptable
but the contribution of high energy positrons (i.e., insufficiently remoderated positrons) should be taken into account for further discussion.
Finally, positron annihilation lifetime spectroscopy
was examined by optimizing a positron pulsing andmeasurement systems. Trial measurements for Kaptonand crystalline Si samples were successfully performed.
In summary, transport and measurement performanceof the KUR slow positron system was evaluated with apositron beam during the KUR operation. The brightness enhancement system and positron lifetime measurement system were confirmed to be effective.
5()(5(1&([1] Y. Kuzuya et al. J. Phys. Conf. Series 791 (2017)012012.

31P12-1

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E

10 mm

10 mm
25.4 mmFig. 1 Beam spot images before (a) and after (b)brightness enhancement.

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T. Toyama, Y. Hatano, C. Zhao, A. Yabuuchi, A. Kinomura, K. InoueDQG Y. Nagai,QVWLWXWHIRU0DWHULDOV5HVHDUFK7RKRNX8QLYHUVLW\
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Tungsten (W) is a primary candidate material for theplasma-facing components (PFCs) due to its high melting
point and high sputtering resistance to energetic particles.
Furthermore, the very low solubility of hydrogen isotopes
in W is a notable advantage in reducing tritium (T) retention during the operation of fusion reactors. However, recent studies have reported that neutron-irradiation and ionirradiation cause significant enhancement of hydrogen isotope retention in W, due to hydrogen trapping at irradiation-induced defects such as vacancies, vacancy clusters,
and dislocation loops. Recently it was found that the addition of rhenium (Re) to W drastically reduces the hydrogenisotope accumulation [1]. As a mechanism for this, quantum chemical calculation has been performed [2]; it is suggested that Re is strongly bound to interstitial atoms, sothat recombination of interstitial atoms and vacancies is
promoted, and the formation of vacancy-type defects that
become hydrogen capture sites is suppressed. However, no
experimental studies on this has been obtained.
In this study, we performed electron-irradiation to introduce only a simple Frenkel pair to W or W-Re alloy. The
effect of Re addition on the defect formation is investigated by the positron annihilation method.

irradiation. This implies an existence of defects before irradiation. ĲDYH after electron-irradiation was 162 ps, only 4
ps longer than that for W-5%Re before irradiation. Remarkable increase of ĲDYH was not observed after irradiation.
Different from the case of pure W, the lifetime spectrum
was well fitted with one component both even after irradiation, and Positron trapping at mono-vacancy was notclearly observed. The possible candidate for positron trapping site for W-5%Re after irradiation could be dislocations in which positron lifetime value may be shorter thanmono-vacancy. Other candidate could be vacancy-Re
complexes, however, positron lifetime value at vacancyRe complex might be almost same as at mono-vacancy in
W because Re and W are the “neighborhood” in the periodic table. Further studies by chemical analysis of positronannihilation sites with coincidence Doppler broadening
measurements are now in progress to discuss electron-irradiation induced defects in W-Re.

(;3(5,0(176Electron-irradiation to pure W and W-5%Re (inweight %) was performed at LINAC at KUR at 8 MeV, attemperature of < 100 Υ to the fluence of about 5E+23 e/m2. Positron annihilation measurements (lifetime measurement and coincidence Doppler broadening measurement) were performed.
5(68/76Figure 1 shows results of positron lifetime measurement before and after electron-irradiation for pure W and
W-5%Re. Calculated values of positron lifetime at W bulk,
mono-vacancy in W and di-vacancy in W are also shownby dashed lines. In pure W, the average lifetime, ĲDYH, wasabout 120 ps before electron-irradiation, which is close to
the value in W bulk. After electron-irradiation, ĲDYH wasabout 140 ps, showing positron trapping to vacancy-type
defects induced by electron-irradiation. The lifetime spectrum after irradiation was analyzed with two components;
the shorter component, Ĳ, and the longer component, Ĳ. Ĳ
was 215 ps, suggesting positron trapping at mono-vacancies and/or di-vacancies.
In W-5% Re alloy, ĲDYH before electron-irradiation was
158 ps, longer than that for pure W before electron-

Fig. 1. Results of positron lifetime measurements for pure
W and W-5Re alloy; before electron-irradiation (Unirrad.)and after electron-irradiation (As-irrad.).
5()(5(1&(6>@ Y. Hatano et al., Nucl. Mater. Energy  (2016) 93.
>@ T. Suzudo, A. Hasegawa, Sci. Rep.  (2016) 36738.

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samples used in the first experiment, which were left atroom temperature for approximately 14 days, were subjected to the second hydrogen charging. 

K. Sato, Y. Kondo, M. Ohta, Q. Xu1, A. Yabuuchi1DQGA.
Kinomura1*UDGXDWH6FKRRORI6FLHQFHDQG(QJLQHHULQJ.DJRVKLPD8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The structural materials of spallation neutron sources (SNS) cause more serious
irradiation damage than fission reactors due to highenergy protons or spallation neutrons and the formationof extremely larger amount of gas atoms by nuclear
transmutation [1, 2]. Therefore, irradiation resistance isrequired. Reduced activation ferritic/martensitic steel
F82H, one of the can-didates for fusion reactor structural
materials, has good thermal and mechanical properties[3]. Using this steel, many researchers have investigatedthe effect of He or H on its microstructural evolution [4í6]. The increase in hydrogen retention caused by theinteraction with defects has an influence on themechanical properties of structur-al materials [7, 8].
Vacancy-type defects are detected well by positronannihilation spectroscopy (PAS). Sato et al. determinedthe change in the positron annihilation life-time (PAL)
through experiments and simulations [9]. Comparisonand estimation of the number of hydrogen atoms trappedat single vacancies in electron-irradiated tungsten by PAS
were performed [9]. In this study, the quantity ofhydrogen atoms trapped at vacancy clusters in electronirradiated F82H will be estimated by PAS.
(;3(5,0(176Reducedactivation
ferritic/martensitic steel F82H IEA heat was used. Samples
with diameters of 5 mm were cut from 0.4 mm-thicksheets using a wire electric discharge machine. Samples
were irradiated with an 8 MeV electron linear accelerator
from the Institute for Integrated Radiation and Nuclear
Science, Kyoto University. The irradiation temperature
was 333 ± 10 K, and the irradiation dose was 2.74×1027/m2 (1.75×10-4 dpa). Cathodic electrolysis charging was
performed in an aqueous solution of 0.1 mol/L NaOH
with the addition of 0.5 mass% NH4SCN. The current
density, temperature, and time for hydrogen charging
were 50 A/m2, 303 K, and 4 h, respectively. After hydrogen charging, the sample surface was mechanically polished using polishing paper #2400. Subsequently, samples were soaked with liquid nitrogen within 5 min fromthe end of hydrogen charging. The PAL measurements
were conducted at a liquid nitrogen temperature of 77 K
using a fast digital oscilloscope with a time resolution of
150 ps, i.e., full width at half maximum (FWHM) [11].
The PAL spectra were accumulated with a total count ofapproximately 3×106 and analysed using the PALSfit
package [12]. Isochronal annealing for 0.5 h was conducted every 25 K from 123 to 298 K. Subsequently, isothermal annealing was also conducted at room temperature (298 K). To investigate the repeatability, the same5(68/76 As dislocations, packet/block/lath boundaries, and precipitates exist in unirradiated F82H, a Ĳ1 of
140 ps, which denotes the PAL of dislocations [13], wasfixed. After electron irradiation, a Ĳ2 of 254 ps was obtained. This PAL is almost the same as the calculated PAL
of vacancy clusters composed of five vacancies (V5). After hydrogen charging, Ĳ2 decreased to approximately 230
ps, and was constant until isochronal annealing at 273 K.
After isochronal annealing at 298 K for 0.5 h, Ĳ2 started toincrease during isothermal annealing for 1 h, 2 h, and 4 h,
and was higher than the value before hydrogen charging(254 ps). When the isothermal annealing time reached 8 h,
Ĳ2 decreased to the value before hydrogen charging. Almost the same trend of the change in PAL was observedin the second experiment. The cause of the increase in the
PAL after annealing at 298 K from 0.5 to 4 h cannot be
identified; therefore, it will be investigated in the near
future.
From the theoretical estimation, the number of hydrogen atoms trapped at V5 of 14.5 (ș = 0.805) is obtained. After the first and second hydrogen charging, thePAL decreases by 22 ps and 18 ps, respectively. Compared with the calculated result, each V5 contains 4 hydrogen atoms (ș = 0.22). This value is significantly lower
than the theoretical value. Analysis of the PAL spectra
without fixing Ĳ1 of 140 ps was also performed, because it
is better to obtain a stable PAL. The difference in the PAL
between before hydrogen charging and after annealing at
148 K for 0.5 h was more than 50 ps. In this case, morethan 14 hydrogen atoms can be trapped at each V5.
However, both Ĳ1 and Ĳ2 significantly change in eachtreatment. As F82H contains a variety of positron trapping sites such as dislocations, interfaces of precipitates,
packet/block/lath boundaries, and vacancy clusters, identification of the positron trapping sites may be difficult in
F82H. For future studies, samples with a different number of hydrogen atoms trapped at vacancy clusters will be
prepared, and PAL spectra of F82H will be carefully analysed.
5()(5(1&(6>@ Y. Dai, G.S. Bauer, J. Nucl. Mater. (2001) 43.
>@ Y. Dai HWDO, J. Nucl. Mater. (2005) 33.
>@ M. Tamura HWDO., J. Nucl. Mater. í (1986)1067.
>@ X. Jia, Y. Dai, J. Nucl. Mater.  (2003) 207.
>@ Z. Tong, Y. Dai, J. Nucl. Mater.  (2009) 258.
>@ Z. Tong, Y. Dai, T J. Nucl. Mater.  (2010) 43.
>@ H.K. Birnbaum, P. Sofronis, Mater. Sci. Eng. A (1994) 191.
>@ M. Nagumo HWDO, Metall. Mater. Trans. A  (2001)339.
>@ K. Sato HWDO, J. Nucl. Mater.  (2017) 9.

31P12-3‑110‑

7KHHIIHFWRIJDPPDUD\LUUDGLDWLRQRQOXPLQHVFHQFHSURSHUWLHVRIFROOROLGDO6LQDQRFU\VWDOVT. Nakamura, J. Otsubo, K. KuriyamaDQG A. Kinomura1,&ROOHJHRI(QJLQHHULQJDQG5HVHDUFK&HQWHURI,RQ
%HDP7HFKQRORJ\+RVHL8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 Colloidal crystalline silicon (Si)nanocrystals is known to exhibit a size tunable and efficient visible luminescence at room temperature due toquantum confinement effect. Because of its environmental friendliness and earth-abundancy, colloidal Si nanocrystals are a promising material for future light-emitting
devices and biomedical applications. Various fabrication
techniques for colloidal Si nanoparticles have been developed, such as wet-chemical synthesis andhigh-temperature thermal processing. Recently, we developed an efficient formation process of colloidal Si
nanocrystals from porous Si, which is an interconnectedwire-nanostructure assembly, as a raw material with low
energy cost treatments. This process produces a large
amount of colloidal nanocrystals per batch, and thus itallows us to utilize the Si nanocrystals in practical applications.
Optical properties of Si nanocrystals including luminescence properties are strongly affected by surface chemistry [1]. In particular, insufficient surface terminations
causes the notable decrease in the luminescence efficiencies due to the formation of nonradiative centers i.e.,
dangling bonds. Thus, ambient condition is one of themost important key parameters to determine the luminescence efficiency. There are many reports on the effectsof various environments on luminescence properties of Si
nanocrystals. For example, it has been reported that ahighly oxidant condition such as high humidity environment promotes inhomogeneous oxidation as well as removal of terminated spices on the Si nanocrystals andresultantly the decreases in luminescence intensity occurs.
However, the effect of extreme conditions such as highlevel radiation environment on Si nanocrystals luminescence properties is not known.
In this work, we investigate the effect of gamma-ray irradiation on luminescence properties of colloidal Si nanocrystals. The heavy dose irradiation of gamma-ray on thecolloidal Si nanocrystals causes the decrease in photoluminescence intensity. However, we find that, comparing
with compound semiconductor nanocrystals such as
CdSe, the decreasing effect is much weaker.
(;3(5,0(176 The porous Si used was prepared bya chemical etching of bulk Si. After the etching, porous
layer was formed on the wafer surface, and then, samples
were obtained. The formed sample exhibited a weak red
photoluminescence. For preparing the colloidal Si nanoparticles, porous Si were firstly dispersed in an organic
solvent with a quartz cuvette. Then, pulsed laser light at
266 or 532 nm from a Q-switched Nd:YAG laser (Continuum) was irradiated with a pulse duration of 5 ns and arepetition rate of 15 Hz. During laser irradiation, the po-rous Si dispersed in the organic solution were constantly
stirred by a magnetic stirrer. After the pulsed laser irradiation of porous Si, the colloidal solution sample is obtained. Under UV illumination, the colloidal Si nanocrystal solution exhibits red luminescence.
For gamma ray irradiation experiments, we spin-coatedthe Si nanocrystals solution on the Si surface and thecolloidal Si nanocrystal films were obtained. The prepared film samples were irradiated at room temperature
with gamma-rays of 1.17 and 1.33 MeV from a cobalt-60
source of Institute of Integrated Radiation and Nuclear
Science, Kyoto University. The dose rate of the irradiation was 1.771 KGy/h. Total gamma-ray dose was ~150kGy.

PL. intensity (arb. units)35

5

Without irradiation

4
3
2

With gamma-ray
irradiation (150 KGy)

1
0
500

600

700

Wavelength (nm)

800

900

Fig. 1. PL spectra of colloidal Si nanocrystal films
with and without gamma-ray irradiation.
5(68/76 Figure 1 shows PL spectra of colloidal Si
nanocrystal films with and without gamma-ray irradiation.
As shown in the figure, the heavy dose irradiation of
gamma-ray on the colloidal Si nanocrystals causes thedecrease in photoluminescence intensity. This may be dueto the formation of defect centers formed by gamma-ray
irradiation. However, the degree of the intensity decreaseis much smaller than colloidal CdSe nanocrystals where
the origin of the photoluminescence quenching is gamma-ray induced losses of surface ligands [2]. In our previous work, it was shown that Compton electrons emitted
by the gamma-ray irradiation causes lattice defects of
ZnO crystals [3], where the degree of the luminescenceintensity change is trivial in spite of heavily dose. Thus,in the present case, such a Compton effect on the Si coreof nanocrystal is attributed to the photoluminescencequenching.
5()(5(1&(6[1] Dohnalová, K. HWDO J. Phys. Condens. Matter (2014) 173201.
[2] Stodilka, R. Z. HWDO J. Phys. Chem. C  (2009)
2580–2585.
[3] Tashiro, J. HWDO Solid State Commun  (2019)24–26.

31P12-4‑111‑

35

Irradiation technique for study on corrosion resistance of fusion divertor materials
to liquid metal during irradiation

M. Akiyoshi, M. Kondo1DQG A. Kinomura2
Radiation Research Center, Osaka Prefecture University
1.Lab. for Nucl. Reactors, Tokyo Institute of Technology
2Inst. for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION:
Development of divertor material is one of the mostimportant issues for future fusion reactor, where highthermal conductivity in severe neutron irradiation environment, sputtering resistance, and low radioactivity isrequired. Although development of SiC ceramics, tungsten, and its composite material is furthered, neither has
resulted in the solution of this problem.
The liquid divertor is completely different approachfrom the conventional divertor material development, thatis covering a surface of material with coolant liquid metal,
and it can expect to moderate damage to the structurematerial. There is little study on the compatibility of liquid metal and structure material, and furthermore, compatibility study during irradiation is quite limited.
EXPERIMENTS and RESULTS:
In the previous year, it was planned to perform the corrosion experiment after an electron irradiation. However,
it is impossible to avoid corrosion on the surface by underwater or in air irradiation. Therefore, tin (Sn) was
sealed in a small irradiation container (30344mm)
manufactured by SUS316L stainless steel, and inside ofthecontainer,
aluminumrich
ferriticsteel(Fe-18Cr-3.3Al-0.4Si) NTK04L with 100ȝm Al2O3 oxidization coating was enclosed to performed electron irradiation by KURUNS-LINAC that achieved the corrosion
action inner side of the container under irradiation environment.
In this year, at the first MT, NTK04L specimen (pre oxidation 1000Υ 10h) was irradiated during 1.1×105 sec(32.5h) to a dose of 5.8×1019e that corresponds to 2.3
mdpa (for Fe Ed=40keV) and also ODS sp-10 specimen(pre oxidation 1000 Υ 10h) was irradiated during
1.1×105 sec (32.5h) 6.5×1019e that corresponds to 2.6
mdpa. With this irradiation, rear heat sink was rather
small to make a difference small between front side andrear side temperature. However, for the first specimen,
temperature at the front-side was increased to 500Υ
while at the rear-side was only 300Υ. In the case of thesecond specimen, air blower was settled at the front side
while it was settle rear side at the first specimen. With
this treatment, temperature at the front side was same

500Υ but rear side was kept 400Υ.
At the second MT, FeCrAl-ODS specimen was irradiated in Pb-Li liquid metal during 1.1×105 sec (32.5h) to adose of 6.6×1019 e that correspond to 2.6 mdpa, and also
JLF-1-SS430 specimen was irradiated in Pb-Li during
1.1×105 sec (32.5h) to a dose of 6.8×1019e that corresponds to 2.7 mdpa.
In this irradiation, temperature measurement was failed
because of failure of several AD8495 thermo-couple amplifier IC. Only rear-side temperature was measured andkept it to 370Υ, but after the irradiation, some liquid
metal was over spilled from the container.
To measure the electron current, the specimen holder
was connected to current meter and not connected to
ground directly and also thermo couple was not connected to ground to measure electron current. It is betterto connect the thermocouple to ground with temperature
measurement, and disconnect them when current measurement is performed.

Fig.1 Cu heat sink and retention plate used for the electron irradiation. The irradiation container was placed between heat sink and the retention plate.

Fig. 2 In the second MT, over heat was assumed andsome liquid metal was over spilled from the container.

31P12-5‑112‑

35 Measurement of Positron Lifetimes of Various Diamond-like Carbon Thin Films
K. Kanda, F. Hori1, A. Yabuuchi2 and A. Kinomura2
Laboratory of Advanced Science and Technology for Industry, University of Hyogo
1
Department of Materials Science, Osaka Prefecture
University
2
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: Diamond-like carbon (DLC) film,
which is amorphous carbon film consisting of carbon andhydrogen, has several excellent properties, such as highmechanical hardness, chemical inertness, low frictionalcoefficient, and abrasion resistance [1]. The film properties of DLC film is depended on its three kinds of structural factors, that is, sp2/sp3 ratio of carbon atom, hydrogen content, and free volume [2]. Free volume in the
DLC film has been macroscopically evaluated as film
density, but microscopic discussion on it has not been
carried out yet. In the present study, free volume in the 4kinds of DLC films, which were synthesized by various
deposition methods and deposition conditions, was discussed on the results of positron annihilation spectroscopy (PAS). We also measured the nano-indentation hardness of these DLC films. Indentation hardness is expected
to decrease as quantity and the size of the free volume
increase.
EXPERIMENTS: We prepared 4 kinds of DLC films
for the present study. The first DLC film was depositedby using a plasma-enhanced chemical vapor deposition(PE-CVD) method. On the present plasma condition,hydrogen-rich soft DLC film is expected to be deposited.
The second DLC film was prepared by the ion plating(IP) method, which is very familiar to the industrial field
as a hard protective coating. Last DLC films were is synthesized by filtered cathodic vacuum arc (FCVA) method.
Two kinds of DLC films were deposited using thismethod with the different bias voltage, 100 and 400 V.
All DLC films were deposited on Si wafer with the film
thickness of several hundred nm. Indentation hardness ofthese DLC films was estimated by using a nano-indenter.
PAS measurement was performed at the slow positron
beam system (B-1) at Kyoto University research Reactor(KUR). Doppler broadening profiles of annihilation
J-rays were obtained using a Ge detector for each positron energy. The-low momentum part of spectra wascharacterized by the line-shape S parameter, which isdefined as the number of annihilation events over therange of 511 r 0.80 keV. S parameters as a function ofenergy (S-E curves) were measured in the range of 0 30 keV. Positron annihilation lifetime spectroscopy(PALS) was performed at an energy of 2 keV, corresponding to the DLC film on Si. Figure 1 shows lifetime spectra for the DLC films formed by the FCVA
method. A Kapton (polyimide) film was measured before
and after measurements of the DLC samples as a control
sample. Obtained lifetime spectra were analyzed by the
PALSfit code assuming one-lifetime component.

RESULTS: Experimental results obtained from PAS
measurements were summarized in Table with indentation hardness. Relative S parameter of each DLC film
was obtained in comparison with that of and Si.

Fig. 1 Lifetime spectra for the DLC samples
formed by the FCVA method with different bias
voltage.
Table 1. positron lifetime and S parameter obtained
from PAS measurements with nano-indentation
hardness of each DLC films

The DLC film, which is synthesized by the FCVA method with the bias voltage of 100 V, has very high indentation hardness and its positron lifetime and relative S parameter are smaller than those of other DLC films. The
DLC film deposited by the PE-CVD method, which has
low hardness, has a large positron lifetime and relative S
parameter. As described above, positron lifetime decreases with increasing hardness. The relative S parameter also shows a tendency similar to a positron lifetime,
but does not completely agree. PAS techniques give information on voids consisting of the free volume. It
should be noted that positron lifetimes reflect void sizes
but S parameters reflect void densities in addition to void
sizes. We think that the hydrogen in the DLC film influenced the results of the S parameter. We are planning toobtain the hydrogen content and the sp2/sp3 ratio of carbon atom in these films by measuring elastic recoil detection analysis (ERDA) and near-edge x-ray fine structure(NEXAFS), respectively.
REFERENCES:>@ S. Aisenberg et al., J. Appl. Phys.  (1971).
>@ J. Robertson, Surf. Coat. Technol.  (1992).

31P12-6‑113‑

35

Positron annihilation spectroscopy on diamond-like carbon films

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Innovative Functional Materials Research Institute, National Institute of Advanced Industrial Science and Technology
1Institute for Integrated Radiation and Nuclear Science,
Kyoto University

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>@ 6 1DNDR et al. .855, 3URJUHVV 5HSRUW 
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in &(7)/7 and U(7) (Fig. 1). These results strongly suggest that a crossover of the low-7 states between FL and
NFL occurs around [*. Together with our high-pressure
U(7) measurements for some concentrations, we suggestthat the anomalous metallic state in UBe13 is mainly ascribed to the inter-U-site electronic correlations. We plan
to make further detailed discussion by checking the Uconcentration [ using ICP-MS at the Institute for Integrated Radiation and Nuclear Science, Kyoto University.

Fig. 1. The U concentration dependence of the characteristic temperatures 7*F and 7FLU, below which F and U
show a tendency to behave like Fermi liquid, respectively.
$&.12:/('*(0(17
We are grateful to Dr. J. Prchal for his assistance in the
low-temperature experiments. The present work was
supported by JSPS KAKENHI Grant Number
JP15H05882, JP15H05885 and JP15K21732 (J-Physics),
and the Strategic Young Researcher Overseas Visits Program for Accelerating Brain Circulation from the Japan
Society for the Promotion of Science. The Prague groupwas supported by the Czech Science Foundation by the
Grant No. P204/15/03777S.
5()(5(1&(6>@ H. R. Ott, H. Rudigier, Z. Fisk, and J. L. Smith,Phys. Rev. Lett. 50 (1983).
>@ S. Yotsuhashi, K. Miyake, and H. Kusunose,- Phys. Soc. Jpn. 71 (2002).

31P13-2‑118‑

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T. Suzuki1, Z. Ma1, S. Fukutani2 and T. Yamamura2

and 0.1 ppb, and lank. The upper limitation of sample
concentration which can be feed into this ICP-MS is defined as 1 ppb. The repetition of measurements is 5.

'HSDUWPHQWRI1XFOHDU6\VWHP6DIHW\(QJLQHHULQJ
1JDRND8QLYHUVLW\RI7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The accurate and precise analysesof actinides and many kinds of fission products in the
spent fuels and/or nuclear debris are important issue fornuclear fuel management and the radioactive waste management. The separation or removal of the actinides isrequired before the above analyses. Especially, for thequantitative actinide analysis and the actinide isotope
ratio analysis by using mass spectrometry such as
ICP-MS (inductivity coupled plasma mass spectrometry)or TIMS (thermal ionization mass spectrometry), themutual separation of actinides is highly important fromthe viewpoint of removal of isobaric interferences. And
also, for the analyses of fission product nuclides, the removal of uranium and plutonium, which are dominantelements in the spent fuel or nuclear debris, is important.
We have been studying the separation and removal ofactinides by using the solid type absorbents such asamine type resin, amino type resin. By the way, the lightactinides have many valences, and the adsorption behaviors of actinides on solid adsorbents depend on their valences. We must study the adsorption behaviors of eachvalences of actinides on solid adsorbents. For this study,
the control and confirmation of actinide valences, theadsorption experiments, and the detection and measurement methods of actinides are necessary. However, now,the preparation for application of actinides in Institute forIntegrated Radiation and Nuclear Science (IRNS), Kyoto
University, has not been readied enough to carried out theexperiment. In consideration under such a situation, we
confirmed the fundamental characteristics of ICP-MS set
in hot laboratory of IRNS.

5(68/76 Mass spectrum around mass number of
151 and 153 is shown in Fig. 1. The good peak curves on
151 and 153 are obtained. Although peak points are little
difference from the real mass, the peaks are corrected bymass calibration.
The relationship of europium sample concentration andcps is shown in Fig. 2. We confirmed that the cps of concentration of 0.1 ppt is same level of background..
We confirmed the generation of molecular ions; hydrateion, monoxide ion. We didn’t observed the dioxide ion.
The generation ratios of molecular ions and atomic ion
are about 10-3. However, the cps of every detected molecular ion was so small that we should carry out further
precise measurement.

,&306 (;3(5,0(176 We use the ICP-MS (Analytik jena, Plasma Quant MS) set in a hot laboratory of
IRNS. The standard solution of europium for ICP-MS(AccuStandard Inc.) was used as the sample. The lanthanides are one of the targets of our study. Some lanthanides are mono-isotope elements, and some lanthanides
have many isotopes. Europium has two isotopes; 151Eu
and 153Eu. Number of isotopes is appropriate, because of
not too many. It is also desirable that the mass number sof isotopes are alternate, that is, if the mass numbers arecontinuous, it is difficult to distinguish the mass of theheavier isotope ion and the mass of hydrate ion of lighter
isotope. The confirmations in this year are the spectrum
profile, the detection limitation, and the generation ofmolecular ions. The concentration of europium for the
spectrum profile and the molecular ion generation was 1
ppb, and for the detection limitation was 1ppb, 10 ppt,

31P13-3‑119‑+5[u10 ]
3
CPS



2
1
0
150

151

152

153

Mass
Fig. 1. Mass spectrum of europium by ICP-MS

5

10

4

10
CPS

35

3

10

2

10

Blank
-2

10

0

10

2

10

Concentration of sample / ppt

Fig. 2. Relationship of europium sample concentration and cps. Solid circles and open circles are dataof 151Eu and 153Eu, respectively. Datum of blanksample was set on 10-2 ppt.

35

3UHSDUDWLRQRI5D$FVWRFNVROXWLRQK. Shirasaki, H. Kikunaga1, K. Washiyama2, A. Shinohara3, T. Yoshimura4, K. Nagata4, C. Tabata5, and T.
Yamamura5,QVWLWXWHIRU0DWHULDOV5HVHDUFK7RKRNX8QLYHUVLW\
5HVHDUFK&HQWHUIRU(OHFWURQ3KRWRQ6FLHQFH7RKRNX8QLYHUVLW\$GYDQFHG&OLQLFDO5HVHDUFK&HQWHU)XNXVKLPD0HGLFDO
8QLYHUVLW\
'HSDUWPHQWRI&KHPLVWU\*UDGXDWH6FKRRORI6FLHQFH
2VDND8QLYHUVLW\
5DGLRLVRWRSH 5HVHDUFK &HQWHU ,QVWLWXWH IRU 5DGLDWLRQ
6FLHQFHV2VDND8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In the past decade, 225Ac (71/2 = 10d) which decays through a chain of four α-emissions andtwo β-emissions to the stable 209Bi, has been receiving
constant attention as a targeted alpha therapy (TAT) nuclide due to its ability to kill considerably high efficiencyof tumor cell [1]. By contrast, γ-rays of 225Ac suffer fromlow emission ratios and are often unresolved from the γemissions associated with its daughter nuclides. Thus γray spectrometry, which is a convenient method for identification of radionuclides, has an uncertainty about the application to 225Ac. This fact makes it difficult to study
chemical properties of actinium complexes using a tracer
amount of 225Ac.
In terms of emission ratios of γ-rays, 228Ac (71/2 = 6.15
h, daughter nuclide of 228Ra) has potential value because it
emits well-defined and intense γ-rays that are easily resolved from the daughter nuclides. Aldrich HWDO reported
the preparation method of 228Ac generator from natural
thorium salts in 2020 [2]. Their method was composed of
two parts with the balk thorium separation by the precipitation of thorium hydroxide, and purification of 228Ra by
the column chromatography using ion-exchange resins. In
the handling of thorium hydroxide, the voluminous slurry
precipitate complicates the convenient separation from thedaughter nuclides.
Hence, we studied simple bulk thorium separation bycation exchange chromatography.

which was preconditioned with a 1 M (mol/L) citric acidsolution. The eluate from the column was collected (fraction 1), then an additional 1 M citric acid solution was
passed through for washing the column (fraction 2 andfraction 3). The column was then washed with 0.1 M
HNO3 to remove residual citric acid (fraction 4) andflowed 6M HNO3 (fraction 5). These fractions were subjected to the γ-ray spectrometry using a high-pure Ge-detector (ORTEC). The 228Ac activity was determined by γemission of 911 keV. The distribution ratio ('i) of 228Ra ineach fraction (L = 1-5) was calculated by the equation:(1).
     
Here, $i is an activity obtained from γ-ray spectrometry of
fraction L.
5(68/76 As shown in Fig. 1, almost all of 232Th
daughters were found in fraction 1, which was assumed tobe contained thorium as a major eluted nuclide. 

Fig. 1. γ-ray spectra of a sample of fraction 1.
The initial 228Ra atomicity (11) of each fraction can be estimated by the equation:            (2).
Here, 12 and 12’ are the number of 228Ac atom at initialand elapsed time W, respectively, λ1 and λ 2 are the decay
constant of 228Ra and 228Ac, respectively. The distribution
ratios (') of 228Ra in the fractions 1-5 were determined by
228(;3(5,0(176 The separation method was based ona technique used in conjunction with 223Ra separation from
irradiated thorium [3]. Thorium oxide was dissolved inconc. HNO3 spiked with a slight amount of conc. HF withheating (~230°C) for approximately 5 min. The solution
was evaporated near dryness and added mili-Q water (18.2
MΩ, repeated two times). Then, the solution was broughtto dryness and reconstituted in mili-Q water with citricacid. Finally, the solution volume was adjusted by the addition of mili-Q water.
The thorium citrate solution was processed according to
the following steps. The solution passed through an ion exchange column containing 2.5 mL cation exchange resin,

Ac activities and summarized in Table 1. This result indicates that approximately 40% of 228Ra is remained inbulk thorium.
Table 1 228Ra distribution ratio (') in the separation steps
Fraction no.
1
2
3
4
5
'
0.431 0.075 0.001 0.005 0.489

5()(5(1&(6[1] C. Kratochwil HW DO, J. Nucl. Med.,  (2016) 19411944.
[2] K. E. Aldrich et al., Inorg. Chem.,  (2020) 3200-3206.
[3] T. Mastren HWDO, Scientific Reports,  (2017) 8216.

31P13-4‑120‑

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M. Nogami1 and T. Yamamura2
1)DFXOW\RI6FLHQFHDQG(QJLQHHULQJ.LQGDL8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\

2,1752'8&7,21 Development of highly selective
compounds for actinyl ions has been important. We
have been focusing on monoamide compounds as promising candidates, considering the possibility of complete
incineration of waste compounds (so-called “CHON
principle”[1]). This year, as the first year of the project,
we made a summary on various monoamides we havebeen investigating. In addition, some subjects whichshould be investigated during the next few years and environments necessary for experiments to be carried out in
KUR were extracted.
5(68/76  0RQRDPLGHFRPSRXQGV We have clarified that adsorptivity of various synthetic organic resins
with a monoamide structure as the functional group touranium(VI) species in acidic nitric acid solutions greatly
differs depending on the chemical structure of the functional monoamide[2,3]. There seems to be two factors
for interaction between monoamides and actinyl ions;
one is “chelating effect” of the ring formed by polymer
monoamides and actinyl ion(s), and the other is “flexibility” of monoamide.
For chelating effect, it is well known that five- or
six-membered rings are most stable for common metal
complexes. While, situation seems different for our
resins. For example, polymerized dimethylacrylamide(DMAA), one of resins with high adsorptivity and selectivity for U(VI) in HNO3, is expected to form
eight-membered ring when it adsorbs U(VI) (UO22+),
where five carbon atoms and two carbonyl oxygen atomsof two DMAA molecules, and one uranium atom arecomposed of the ring (Fig.1)[2]. In addition, eight
would be the minimum number for the chelating ring
formed by our synthetic resins. These things suggestthat detailed investigations on cheating effect for resins
with a larger ring than common complexes are necessary.

functional group and the main polymer chain. Flexibility would be very effective in case that adsorption occurs
by, HJ, ion exchange, namely, the approach of pluralions with positive and negative charges, respectively.
On the other hand, for monoamide resins, two monoamide carbonyl groups are in general necessary to capture
one UO22+ ion, as can be seen in, e.g., Fig. 1. Effect of
flexibility of monoamide resins might be, therefore, suppressed compared with that of ion exchange resins.
Moreover, functional groups with longer chains must be
disadvantageous from the viewpoint of chelating effect,
because the number of atoms consisting of chelatingrings becomes larger as mentioned above.
We have been accumulating adsorption data of ourmonoamide resins for U(VI), but we have not found any
clear tendency between the chemical structure of functional monoamide and the adsorptivity. We have also
take into account the fact adsorption of U(VI) by monoamide resins occurs not only at oxygen atom of monoamide but also at other sites, which was clarified by the
Scatchard plot analysis[4].
 )XWXUH VWXGLHV IRU PRQRDPLGH FRPSRXQGV  Theabove things were examples on resins. Current status
for the development of our monoamide resins was introduced at the symposium held at KUR on Feb. 7, 2020,and fruitful discussions were made.
We have also been developing monoamide extractants
and precipitants as well as resins. Based on the above
knowledge, we will carry out the following studies at
KUR.
Experimental areas treating actinide species are underpreparation. Determination of concentration of actinide
species is essential for our study, and an ICP-MS instrument has been introduced. We would like to establish
the determination condition for ICP-MS with our colleagues.
Theoretical approach would also be necessary for understanding the interaction between monoamide compounds and actinyl ions. We would like to make frequent discussions with our colleagues in this regard.
5()(5(1&(6[1] M. G. B. Drew HWDO, Dalton Trans. (2007) 244-251.
[2] M. Nogami HW DO, J. Radioanal. Nucl. Chem., (2007) 37-41.
[3] M. Nogami HW DO, Prog. Nucl. Energy,  (2008)
462-465.
[4] M. Nogami HW DO, J. Radioanal. Nucl. Chem., (2010) 541-546.

Fig. 1. Expected bond style between DMAA resin andUO22+ Flexibility is somewhat an opposite relationship tochelating effect. Functional groups are expected to improve the ability to capture metal ions more easily withan increase in flexibility, LH, the length between the

31P13-5‑121‑

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&RQVLVWHQF\YHULILFDWLRQEHWZHHQUHODWLYLVWLFTXDQWXPFKHPLFDOFDOFXODWLRQVDQGH[SHULPHQWVLQXUDQLXPFRPSRXQGV

M. Abe1, M. Hada1, A. Sunaga1, A. Sato1, T. Yamamura2,
C. Tabata2
'HSDUWPHQWRI&KHPLVWU\7RN\R0HWURSROLWDQ8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Theoretical calculations of actinide compounds are very important to understand or predict new phenomenon in these compounds. We have developed computational methods based on the relativistic
quantum chemistry and applied it to uranium (U) isotope
fractionation, which is widely discussed in geochemistry[1]. In the present work, we evaluated equilibrium isotope fractionation coefficients (H) for 54 U species in
U(VI), U(V), and U(IV) states with various ligands (e.g.,
H2O, CO32-, CH3COO-, Cl-, NO3-, etc.) using accurate
relativistic quantum chemical methods to verify the accuracy of the computational results and predict Hfor new
species.

Fig. 1. ln.nv, ln.nm, and H of 54 U species. The light
blue, green, and deep blue plots represent H, ln.nv,
and ln.nm, respectively. These plots for U(VI), U(V),and U(IV) species are surrounded by the purple, orange, and pink rounded squares, respectively. [6]0(7+2'6 We calculated H between 235U and 238U as
the sum of the nuclear volume term (ln.nv) and the nuclear mass term (ln.nm) [2-4]. ln.nv is due to the electronic energy difference caused by the different size andshape of nucleus of isotopes [2,3], while ln.nm is due tothe vibrational level caused by the different reduced massof isotopologues [4]. In the heavy element system, ln.nv
is dominant in H. Because ln.nv is highly affected by relativity, we used the exact two-component (X2C) relativistic method with the Gaussian finite nucleus model, implemented in the DIRAC16 program.
5(68/76 As a calibration, we calculated H for
U(IV)-U(VI) in chlorides and obtained as 1.72‰, which
agrees well with the experimentally reported H (1.64‰)[5]. As shown in Fig. 1, H strongly depends on the uranium valence state, and its general order is U(VI) > U(V)
> U(IV). Also, we can confirm that the magnitude ofln.nv is much larger than ln.nm from Fig.1. This is consistent with the fact that ln.nv is the dominant term in U
isotope fractionation. To explain the strong dependenceof H on U valence, we depicted the radial distributionfunction of 6V orbital of U6+, U5+, and U4+ atomic ions(Fig. 2) because this orbital significantly affects the magnitude of ln.nv. The order of spread of 6V orbital is U6+ <U5+ < U4+, indicating that 6V orbital is more spread as
more 5I electrons are added. This causes the decrease inelectron density at the nucleus, leading to the large ln.nv[3], and consequently, H shows large value. Besides, thelargest difference in H between U(VI) and U(IV) is about3‰, which indicates that the U speciation significantly
affects isotope fractionation. The present theoretical data
set of H including various specification would be very
helpful for the accurate discussions of U isotope fractionation in geochemistry.

Fig. 2. Radial distribution function of 6s orbitals in
U6+, U5+, and U4+ atomic ions. Purple, orange, andpink lines represent the functions of U6+, U5+, andU4+, respectively. Electronic configuration of theseions are shown in the red box. [6]5()(5(1&(6[1] C. H. Stirling HWDO, Geochim. Cosmochim. Acta, (2015) 200-218.
[2] M. Nomura HW DO, J. Am. Chem. Soc.,  (1996)
9127-9130.
[3] J. Bigeleisen, J. Am. Chem. Soc.,  (1996)
3676-3680.
[4] J. Bigeleisen and M. G. Mayer, J. Chem. Phys., (1947) 261-267.
[5] Wang HW DO. Geochim. Cosmochim. Acta, , 262(2015)[6] A. Sato, R. Bernier-Latmani, M. Hada, and M. Abe, tobe submitted.

31P13-6‑122‑

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H. Shishido, H. Hashizume, C. Tabata1DQG T. Yamamura1*UDGXDWH6FKRRORI(QJLQHHULQJ7RKRNX8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
Partitioning and transmuting
is presently regarded as an effective method to address
the issue of high-level radioactive waste disposal. The
most efficient way to transmute minor actinide (MA)
nuclides is to cause fission reactions with neutrons, andsuch stud-ies have been reported since almost the
beginning of the use of nuclear energy [1]. Neutrons
generated by fusion reactors are most preferred fortransmutation because of their high energy andmonochromaticity. We have pro-posed to transmute MA
rather moderately, namely with a low fission reaction
rate to avoid imposing severe engi-neering challenges
on the system design [2].
In this concept, MA mixed oxides (e.g., Am–Cm–O)
are loaded into limited space in fusion reactors,
where sufficient neutron flux can be secured withrelatively lower heat flux. Whereas some studies havereported the phase diagram of U or Pu based MA
oxides, no reports have provided the diagrams of theMA-only mixed ox-ides. It is vital to reveal theproperties and construct a database for realization of thetransmutation system.
The objective of this study is to evaluate thephase diagram of the MA-only mixed oxides.
Measurement of the phase diagrams is not astraightforward task because the toxicity, radioactivity,
scarcity and the short lifetime of many actinides impede
experimental studies. Thus, we aim to develop a method
to evaluate the phase diagrams. In the first year, we
discussed the research direction and important issues tobe solved each other. We also exam-ined the phase
diagrams of MA from earlier studies.
',6&866,21 We had a meeting at Research Reactor
Institute in Kyoto University and the concept of this research and important issues have been confirmed eachother. The most focused point was the idea of MA transmutation to Plutonium even number nuclides in the research concept. We have proposed a rather moderatelytransmuting MA in a fusion reactor to reduce the heatgeneration from fission reactions [2], which results in the
production of many Pu-238 nuclides. However, one important issue—the decay heat from Pu-238—was indicated in the meeting. The nuclide Pu-238 has large decay
heat and is utilized as a heat source in radioisotope thermoelectric generators. We have concerned a possibility tohandle the large quantity of the targets having large andcontinuously decay heat in a huge fusion reactor system.
The research direction is still under debate and we proceed with the research from a general point of view tosolve the crucial issue.
5(6($5&+ 5(9,(: The term CALPHAD (CALculation of PHAse Diagram) means calculating phase
diagrams from thermodynamic models with parameters

Fig. 1. Schematic flow chart for the numericalsimulation of the statics of phase transformation [6].
adjusted to available measured data. Few researches haveevaluated the phase diagrams and thermodynamic modelsof the MA mixed oxides (U–Pu–Np–O, Pu–Am–O) [3-5].
These studies were based on very limited experimental
values to derive the thermodynamic models. Unfortunately, there are no thermodynamic data of the MA-only
mixed oxides; thus, ab initio calculation needs to be performed to provide inputs for CALPHAD.
Figure 1 schematically depicts the situation of ab initio with respect to CALPHAD [6]. The ab initio calculation can provide energetics and phase diagram information. The energetics (structural energies, heats formation) of existing or hypothetical compounds can beeasily evaluated and directly input in a CALPHAD database. The ab initio outputs can be also converted to a
Redlich–Kister format and combined with the thermodynamics database in use with CALPHAD. This procedure
has been successfully applied to some cases of binary
metal alloys [7]. We consider that the phase diagrams of
the MA-only mixed oxides can be predicted with a certain accuracy based on the examination above.
)8785(7$6.6 We move forward with the ab initio
calculations to evaluate the energetics of the MA oxides.
It is important, as well known, that the values provided
by ab initio calculations must be assessed critically because the values depend on the methods and approximations used and they scatter similarly to how experimental
values do. Because we do not have expert knowledge thatguarantees the best results for the issues, prudent andcritical study is under way.
5()(5(1&(6>@ S. L. Beaman et al., NR-CONF-001, United States
Nuclear Regulatory Commission, (1976).
>@ Y. Furudate HWDO., Prog. Nucl. Energ.  (2018)28-32.
>@ C. Guéneau HWDO, in &RPSUHKHQVLYH1XFOHDU0DWHUL DOV, edited byR. J. M. Konings (Elsevier, 2012), Vol. 2
[4] M. Hirota HWDO., J. Nucl. Meter.  (2005) 84-88.
[5] P. Gotcu-Freis HWDO., J. Nucl. Mater.  (2011) 408421.
[6] P. E. A. Turchi HWDO., CALPHAD  (2007) 4-27.
[7] L. Kaufman HWDO., CALPHAD  (2001) 419-433.

31P13-7‑123‑35

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will be tested and the synthetic scale will also be enlarged.

/DERUDWRU\IRU$GYDQFHG1XFOHDU(QHUJ\7RN\R,QVWLWXWHRI7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\

,1752'8&7,21  In Th fuel cycle, effective separation of U from Th and other fission products in spent Th
fuels is needed. To enable that, an extraction method similar to plutonium–uranium redox extraction (PUREX) has
been studied, namely, thorium–uranium extraction(THOREX)[1]. In the THOREX process, UO22+ is extracted by tri-Q-butyl phosphate (TBP) with the aid of
Al(NO3)3. Some of the other ligands such as monoamide
is recently reported for U/Th separation [2]. In both thecases, extractability of UO22+ is high, but that of Th4+ isalso high, leading to low selectivity of UO22+ over Th4+.
Therefore, study on highly selective ligands to specificlight actinide is needed. In this study, Phthalocyanine(Pc) was selected as the main structure of the ligand. Pc
is known as forming stable complex with U and there aremany reports on mechanism and characterization study.
However, the Pc has low solubility in organic solvent
which limit the utilization in solvent extraction. Therefore,
the Pc derivatives with substituent modification wasplanned and metal free Pc and Pc-Zn complex were synthesized in fiscal year of 2019. Zinc was selected becauseof the relatively weak interaction of Zn and N of Pc. Oneof the most famous complexes of Pc is Pc-Cu complex
but the covalent bond of Cu and N of Pc is too strong to
exchange to other metal ions. Also, N is easily protonatedunder acidic condition, hence the O-derivatized Pc will
also be synthesized. During this study, applicability of Pc
derivatives to solvent extraction will be surveyed.
(;3(5,0(176 $1' 5(68/76 Synthesis of Pc
was done at Tokyo Tech and test-run of hydrothermal
synthesis of U-complex was done at Koyo University. To
synthesize the Pc, literature survey was firstly done andsome preliminary experiments were conducted. The simple metal free Pc and Pc-Zinc complex were synthesized
as following schemes in (1) and (2) of Figure 1. In boththe schemes, the starting building block of phthalonitrile
can be replaced into derivatized one and the combinationof different building blocks can make the synthesis ofother Pc derivatives easily possible. Also, Zn in the Pc-Zncomplex can be easily replaced into other metals. For
purification of metal free Pc and Pc-Zn, Soxhlet extractor
and thin layer chromatography (TLC) were used respectively. The color of metal free Pc and Pc-Zn were whiteand dark blue, respectively as shown in Figure 2. By
1
H-NMR measurement, successful synthesis of the desired products was confirmed. The purities of both products were not high enough for characterization study,
hence, further purification methods such as distillation)LJXUH  6\QWKHWLF VFKHPH RI   PHWDO IUHH 3F DQG
 3F=Q)LJXUH  3LFWXUHV RI V\QWKHVL]HG FKHPLFDOV   PHWDOIUHH3FDQG  3F=Q)8785(3/$1 From next fiscal year, the following
experiments are planned;
1.Synthesis of Pc derivatives with long alkyl chain to
increase solubility in organic phase.
2.Survey of the synthetic scheme of Pc derivatives-U
complexes.
3.Survey of the synthetic scheme of Pc derivatives tomake the Pc 1,2-hybrid donor ligand
4. Trial of single crystal synthesis of Pc derivatives andsome metals and their characterization&21&/86,216 The synthetic schemes of metal free
Pc and Pc-Zn complex were established and the further
synthetic strategy was made clear. The characterization
study will also be started from next fiscal year.
5()(5(1&(6[1] R.H.Rainey and J.G.Moore, 1XFO 6FL (QJ, 10(4),367–371, 1961.
[2] P.N.Pathak, 6ROY([W,RQ([FK, 20(3), 293–311, 2002.

31P13-8‑124‑

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K. Mori1 and F. Fujisaki2
,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\ .8516 
2IILFHRI6RFLHW\$FDGHPLD&ROODERUDWLRQIRU,QQRYDWLRQ.\RWR8QLYHUVLW\,1752'8&7,21 The all-solid-state rechargeable
battery is a key technology for large-scale applications
such as electric vehicles, plug-in hybrid vehicles, andelectrical energy-storage systems in future smart grids.
The use of solid electrolytes is critical for improving thebattery performance parameters: energy density, power
capacity, lifespan, and reliability. In the last decade,fluoride-ion batteries (FIBs) have attracted much attention as alternative candidates for lithium-ion batteries,
nickel-metal hydride batteries, sodium-ion batteries,and so on. However, no standard choice for FIB materials has been established. For the realization of allsolid-state FIBs, it is very important to explore new fluoride-based solid electrodes and electrolytes. In thiswork, we performed structural studies for fluoride-ion
battery materials such as Cu nanoparticle with BaF2
(hereafter referred to as nano-Cu + BaF2), AlF3 nanoparticle (hereafter referred to as nano- nano-AlF3), AlF3
nanoparticle with Li (hereafter referred to as nano-AlF3+ Li), using the VCND on the B-3 beam port of KUR.
(;3(5,0(176 Powder samples of the “nano-Cu +BaF2”, the “nano-AlF3”, and the “nano-AlF3 + Li” were
put into a cylindrical vanadium-nickel-alloy holder (diameter: 6 mm, thickness: 0.1 mm) under a high-purity
argon atmosphere. ND experiments were performed using the VCND, as shown in Fig. 1. The neutron wavelength, λ, which is monochromatized by the (220) plane ofa Cu single crystal (i.e., Cu monochromator), is 1.0 Å.
Their ND data were collected in the 2θ range of 10–115º at room temperature. In addition, their X-ray diffraction (XRD) data were recorded on an X-ray diffractometer with Cu.Į radiation (λ = 1.54 Å; SmartLab,
Rigaku Co.) at room temperature.
5(68/76 The ND data of the “nano-Cu + BaF2”, the“nano-AlF3”, and the “nano-AlF3 + Li” were shown in
Fig. 2(a). Obviously, Bragg reflections were clearly observed in the higher 2θ range of ND data, comparedwith XRD data (see Fig. 2(b)). It is most likely that the
ND data enable us to offer the precise atomic positions
and thermal factors of F– ions, since the scattering amplitude (or coherent scattering length) of F is as large as
those of other elements. Further analysis (e.g. Rietveld
analysis) is now in progress to determine their structures.
The authors acknowledge Mr. Tanaka of Kyoto University for his help with the sample preparation.

Fig. 1. Versatile compact neutron diffractometer (VCND)
installed at the B-3 beam port of Kyoto University Research Reactor (KUR).
(a)

(b)

Fig. 2. (a) Neutron diffraction data of Cu nanoparticle
with BaF2 (nano-Cu + BaF2), AlF3 nanoparticle (nanoAlF3), AlF3 nanoparticle with Li (nano-AlF3 + Li) collected at the VCND. (b) X-ray diffraction data of the“nano-Cu + BaF2”, the “nano-AlF3”, and the “nanoAlF3 + Li” collected at the X-ray diffractometer with
Cu.Į radiation.

31008

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K. Mori, R. Okumura, H. Yoshino, M. Kanayama, S. Sato1,
K. Iwase2, Y. Oba3, H. Hiraka4, F. Fujisaki5, F. Kobayashi6,
and T. Emoto6(a),QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\ .8516 
+LJK(QHUJ\$FFHOHUDWRU5HVHDUFK2UJDQL]DWLRQ .(. 'HSDUWPHQWRI0DWHULDOVDQG(QJLQHHULQJ,EDUDNL8QL
YHUVLW\
0DWHULDOV 6FLHQFHV 5HVHDUFK &HQWHU -DSDQ $WRPLF (Q
HUJ\$JHQF\ -$($ 
1HXWURQ6FLHQFH&HQWHU.RUHD$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH2IILFHRI6RFLHW\$FDGHPLD&ROODERUDWLRQIRU,QQRYDWLRQ.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\(b),1752'8&7,21 Neutron diffraction is a powerfultool to precisely determine the positions of light elements(e.g., hydrogen and lithium) in solids. This is the main reason why neutron powder diffractometers are critical for
structural investigations of energy storage materials, forexample, rechargeable lithium-ion batteries and hydrogen
absorbing alloys. The B–3 beam port of Kyoto University
Research Reactor (KUR) had long been used as a four-circle single-crystal neutron diffractometer (4CND). For thelast decade, however, the 4CND was so old that its research activity on neutron science was quite low. Now, theversatile compact neutron diffractometer (VCND) is installed on the B-3 beam port of KUR.
63(&,),&$7,216 Figure 1 shows the current state of
the VCND. The neutron wavelength, λ, which is monochromatized by the (220) plane of a Cu single crystal (i.e.,
Cu monochromator), is 1.0 Å. To cover the detector areaof 6 º ≤ 2θ ≤ 130 º, twenty-five 3He tube detectors (1/2 inch
in diameter) are used, where 2θ is the scattering angle. A
detector bank including twenty-five 3He tube detectors isplaced on the arm of the HUBER-440 goniometer. The distance from the Cu monochromator to the sample is approximately 2 m, and the distance from the sample to the detector is 1.2 m.
&5<67$/6758&785($1$/<6,6 Strontium fluoride (SrF2) is a key material for the solid electrolytes of allsolid-state fluoride-ion batteries. The crystal structure of
SrF2 is well-known as the fluorite-type structure, comprising a metal site and a fluorine site: Sr(0, 0, 0) in the 4D site
and F(1/4, 1/4, 1/4) in the 8F site (Wyckoff notation in
space group )PP). To assess the ability of the VCND,
we performed the ND experiment using SrF2 powder. Figure 2 shows the ND data of SrF2 at room temperature. In
the figure, a good fit was obtained between the observedand calculated intensities. The lattice constant, D, was estimated to be 5.85(15) Å.

Fig. 1. Versatile compact neutron diffractometer (VCND)
installed at the B-3 beam port of Kyoto University Research Reactor (KUR): (a) bird’s-eye-view photographand (b) partial view (around the sample stage) of the
VCND.

Fig. 2. The crystal structure refinement of SrF2 using neutron diffraction data collected at the VCND.

31016

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K. Kaneko, R. Motokawa, Y. Oba, K. Mori1 andR. Okumura1
0DWHULDOV6FLHQFHV5HVHDUFK&HQWHU-DSDQ$WRPLF(Q
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6

5

3

Intensity（ 10 counts ）,1752'8&7,21   The vitrification technique with borosilicate glass isused to immobilize high-level radioactive liquid wastes,
which is produced during the reprocessing of nuclear
fuels[1]. The high-level wastes is mixed with the borosilicate glass and melted, that results in forming an oxide. In
order to have a long-term stability, details of this vitrification process are important. Among the constituents,
molybdate tends to precipitate that lowers durability[2].
The segregation of platinoids also cause issues on fabrication[3].
In order to fabricate stable vitrified radioactive waste,
microscopic insights into the structure are required. Neutron diffraction is suitable to structure of the glass as it
can access to high-4 range. In addition, thanks to its hightransmission, the vitrified waste can be investigatedwithout crashing into a powder form. The latter could be
essential to obtain an actual form of the waste.
Since the research reactor JRR-3 has not been in operation for roughly 10 years, the B-3 diffractometer offers
an unique opportunity to perform neutron diffraction withthe monochromatic beam. As a first step, we performed
neutron diffraction experiments to check feasibility to
study the vitrified nuclear waste using the simulated
waste.

4

3

20

40

60

scattering angle 2θ

80

100

120

( degrees )Fig. 1. Neutron diffraction patter of the borosilicate glass for vitrification without simulated
radioactive waste recorded on the B-3 diffractometer. The inset shows a neutron transmission
image for the same sample.

(;3(5,0(176
The borosilicate glass samples with and without simulated radioactive wastes were prepared to have cylindrical form with several diameters ranging from 6 mm to 20
mm. In order to reduce neutron absorption of boron, oneof the main constituent of the glass, enriched 11B was
used.
Neutron diffraction experiments were performed on
the versatile compact diffractometer installed at the B-3
beam port. Neutrons with a wavelength of 1Å are provided by a Cu monochromator. An array of the 3He detectors which covers 25˚ in the scattering angle allows
efficient measurements. The sample was mounted on thecontinuous rotation stage which increases homogeneity.

image proves that a sufficient transmission was obtained
owing to the 11B enrichment, The suppression of the neutron absorption leads to obtain a clear neutron diffraction
pattern shown in the figure, which was taken for a few
hours at 5MW. In addition to first sharp diffraction peakaround 15˚, the higher-order peaks were clearly observed
around 27˚, 52˚ and 83˚ as well. This high quality datawith the high S/N ration should be sufficient for quantitative analysis and is in progress.
The present result demonstrates that the B-3 diffractometer is suitable for the study on the vitrified radioactive waste. We plan to extend our study on the simulated
radioacitive waste with different compositions and fabrication conditions in order to reveal its impact on the
structure in a microscopic scale.

5(68/76
Figure 1 shows a representative neutron diffraction
pattern of the borosilicate glass for vitrification without
the simulated radioactive waste measured on the B-3. The
inset of the figure displays the neutron transmission image for the same sample taken by the CCD camera. This5()(5(1&(6[1] G. Roth, S. Weisenburger, Nucl. Eng. Des. ,197e207 (2000).
[2] S. Morgan HW DO., Mater. Res. Soc. Symp. Proc. ,151e156 (2003).
[3] H. Mitamura HW DO, Nucl. Chem. Waste Manag. ,
245e251 (1983).

31027

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M. Hino1, T.Hosobata2, T.Oda1, Y.Yamagata2, H.Endo3,
N.L.Yamada3, F. Funama4, H.Yoshinaga1, Y. Kawabata1
1,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ .8516 -DSDQ2
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3
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4'HSW1XFO(QJ.\RWR8QLYHUVLW\-DSDQ,1752'8&7,21  Progress of neutron optical devices is very significant. We have established fabrication
method for aspherical focusing supermirror with metal
substrate [1-3]. The metallic substrate is robust and ductile, to which able to fabricate steeply curved surface withhigh form accuracy. It is also applicable to use under highradiation irradiation and high-temperature filed, even at aplace close to the neutron target and moderator. Furthermore, it is possible to fabricate a large focusing mirror by
combining multiple segmented mirrors with mechanicalfastening entailing the usage of screw holes and fixture
tabs. We have solved the problem of required surface
roughness for neutron mirror. The roughness should besmaller than 0.3 nm for high-P supermirror coating. Here
P is the maximum critical angle of the mirror in units ofcritical angle of natural nickel. By using electroless nickel-phosphorus (Ni-P) plating, we overcame the problem
and are establishing fabrication process for asphericalfocusing supermirror. There is still a problem of peelingoff for high-P supermirror coating on metal substratewith steep curvature. In this study, we reported an improvement of higher-P NiC/Ti(SiC) ellipsoidal supermirror. Here the (SiC) means thin interlayers in which
thickness are less than 1 nm. The NiC layers were sandwiched by the SiC thin inter-layers in to reduce compressive stress of layer and to improve interface roughness
possibly.
(;3(5,0(176 We fabricated ellipsoidal metallic
substrates with the Ni-P plating, based on the technology
using ultrahigh precision cutting with correction processing, followed by mechanical precision polishing. The
first precise manufacturing was conducted at a CNC machine for development of neutron optical devices atworkshop of the KURNS. The ultra-precise manufacturing, polishing and cleaning of the metallic substrate wereconducted at RIKEN. The supermirror coating was conducted with ion beam sputtering machine at the KURNS(KUR-IBS) [4]. The neutron experiments were conducted
at CN-3 beam line at the KURNS and the BL16 (SOFIA)
beam port at J-PARC MLF. We have succeeded in fabricated a couple of NiC/Ti ellipsoidal supermirrors inwhich length of 900mm. The semi-major and semi-minor
axes of the ellipsoidal supermirror were 1250 mm and65.4 mm, respectively. The acceptable angle of the minor
axis arc of the ellipsoidal supermirror is 20 degree [5].
We have fabricated P=6.5 NiC/Ti supermirrors in which
total number of layers was 8900, where the half of thelayers were SiC interlayers.

5(68/76 Figure 1 shows reflectivity profiles of neutrons by the P=6.5 NiC/Ti (SiC) supermirror fabricatedby the KUR-IBS. As shown in Fig. 1 (a), the profile by
the supermirror on metal substrate was almost same withthat on a well-polished silicon wafer. There is no big difference for the reflectivity profiles on each metal elements which corresponds to upstream, center, downstream parts shown in Fig.1(b). By using the new layer
structure, we have realized P=6.5 supermirror, which isdifficult even on a flat surface, on a curved surface with asteep curvature. Here the required number of periodic
layers of high-P supermirror increases with the proportional of P, in which principle is well known as Porod’slaw. The number of effective periodic layers of the supermirror was 4450 and it was not much enough numberfor P=6.5 supermirror. It is also still preliminary measurement and we will report more detail in our future
work.

Fig. 1. Neutron reflectivity of m=6.5 NiC/Ti (SiC)
supermirror deposited simultaneously on (a) metal
substrate and silicon wafer. (b) Those on different
metal elements (upstream, center downstream parts).
5()(5(1&(6>@ J.Guo, HWDO, Optics Express 22(2014) 063108.
>@ T.Hosobata, HWDO, Optics Express 25(2017) 20012.
>@ T.Hosobata, HWDO, Optics Express 27(2019)26807.
>@ M.Hino, HWDO, Nucl. Instr. and Meth., (2015) 265.
>@ T.Hosobata, HWDO, JPS Conf. Proc. 22, 011010 (2018)

31109

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M. Kitaguchi, K. Mishima, N. Muto, A. Umemoto,QVWLWXWHRI0DWHULDOVDQG6\VWHPVIRU6XVWDLQDELOLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI6FLHQFH1DJR\D8QLYHUVLW\.RED\DVKL0DVNDZD,QVWLWXWHIRUWKH2ULJLQRI3DUWLFOHV
DQGWKH8QLYHUVH+LJK(QHUJ\$FFHOHUDWRU5HVHDUFK2UJDQL]DWLRQ.(.

,1752'8&7,21  Experiments measuring position
distributions of ultracold neutrons under the earth’s gravitation [1-3] have been carried out to study gravitation or
short-range forces. For those purposes, ultracold neutron(UCN) detectors with high spatial resolution are useful.
Conventional best detectors had resolutions of 1-2 Pm[4,5]. To improve the ability to study gravitation, we
successfully developed a detector with spatial resolutionof less than 100 nm [6] using fine-grained nuclear emulsion [7]. It was fabricated by sputtering a converter layer
with a structure of 10B4C(50 nm)-NiC-C on a side of silicon wafer at KURRI using the ion beam sputtering system (KUR-IBS) and applying the fine-grained nuclear
emulsion with the thickness of 10 Pm on the layer. The
detector can also be used in neutron imaging. In order toobtain position distributions of neutrons with a high accuracy of submicron, a method to connect images between microscopic views with high accuracy is necessary.
We developed a method using microscopic marks formedon silicon substrates for the purpose. In this experiment,
we sputtered a converter layer with a structure of
10
B4C-NiC-C on silicon wafers with those marks, appliedfine-grained nuclear emulsion on them, exposed one ofthem to cold neutrons at J-PARC, and checked the stability of sputtered layer and the emulsion layer. The rest of
the samples were used in an experiment measuring position distributions of UCNs under the earth’s gravitation at
Institut Laue-Langevin (ILL).

(;3(5,0(176 The detectors were fabricated asfollows. The microscopic marks for fine alignment with
their diameter of 1 Pm, a pitch of 50 Pm, and a depth of
0.5 Pm were formed on areas of 10 mm by 70 mm on
single sides of silicon wafers by electron beam lithography at Nanofabrication Platform in Nagoya University.
After that, wafers were cut into the size of 20 mm by 90
mm and washed. Next, layers of 10B4C(200 nm)-NiC(60nm)-C(20 nm) were formed on those wafers at KURRI
using KUR-IBS. After that, fine-grained nuclear emulsion gel was applied on those wafers with final thicknessof 10 Pm at Lab. F, Physics Department, Nagoya University. A detector was exposed to cold neutrons of 1000 m/s
at BL05, MLF, J-PARC. The exposure density was approximately 2.7×107 neutrons/cm2. After the exposure, it
was developed and checked on stabilities of sputteredlayer and adhesion between the layer of the emulsion.
Observation of tracks was also done with epi-illumination
optical microscope at Nagoya University.

5(68/76 Stability of sputtered layer was confirmed
to be enough that the layer did not separate from silicon
substrate after the application of fine-grained nuclear
emulsion and development. Adhesion between the layer
and the emulsion layer was also strong enough that theemulsion layer did not separate from the sputtered layer
during the development. Tracks of alpha particles and 7Li
nuclei from neutron absorption by 10B in the converter
layer were clearly seen as shown in Fig. 1 with an expected density. Marks for fine alignment were also clearly seen as shown in the same figure.

Fig. 1. Microscopic image of the detector after development. Observed tracks are surrounded by red ellipses.
Marks for fine alignment are surrounded by dashed blue
circles. Tracks and marks were clearly seen after development.
Thus, stability and functionality of the detector was confirmed, and the rest of the detectors were used in an experiment for measuring position distributions of quantized UCNs under the earth·s gravitational field at PF2,
ILL, whose analysis is going on.
5()(5(1&(6
415 (2002) 297.
>@ V. V. Nesvizhevsky et al., Nature,4>@ H. Abele et al., Nucl. Phys. A 827, 593c595c (2009).
>@ G. Ichikawa et al., Phys. Rev. Lett. 112, 071101(2014).
>@ V.V. Nesvizhevsky et al., Nucl. Instrum. Methods
Phys. Res. A 440, 754759 (2000).
>@ T. Jenke et al., Nucl. Instrum. Methods Phys. Res. A,
732, 18 (2013).
>@ N. Naganawa et al., Eur. Phys. J. C, 78(2018)959.
>@ T.Asada et al., Prog. Thor. Exp. Phys., 2017 (2017)
063H01.

31135

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&2

0HDVXUHPHQWIRUWKHUPDOQHXWURQFDSWXUHFURVVVHFWLRQVDQGUHVRQDQFH
LQWHJUDOVRIWKH$P QJJ J$PPJ$PUHDFWLRQVS.Nakamura, S. Endo,A. KimuraDQG Y. Shibahara
-DSDQ$WRPLF(QHUJ\$JHQF\
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\,QWURGXFWLRQ Americium-243 has the half-life of 7367 yr[1] and contributes to the production of 244Cm (18.11 yr [1])through neutron capture reaction. The neutron capture
cross-section data of 243Am are important in considering theamount of 244Cm accumulated in spent nuclear fuels. For theprediction of 244Cm production, a difference of 10% between
calculated and experimental values was reported.[2] Thus theneutron capture cross sections of 243Am were measured bya neutron activation method.
([SHULPHQWV   Nitric acid solutions of 243Am equivalent to 1 kBq were dropped onto fiber filters and dried. To
monitor neutron fluxes, a set of Au/Al and Co/Al alloy
wires was attached to the Am sample as an irradiation
target. Neutron irradiation was performed using irradiation
systems of the KUR. Gamma- and alpha-ray spectrometry
were applied to measurements of irradiated samples.
First, for the 243Am(n,J)244gAm reaction, measurementsof emission probabilities of J rays emitted from the groundstate 244gAm (10.1 h[1]) had been performed under the
project 25P1-16 in 2014. The previous 29% uncertainty[3] in the emission probability had been improved to 2%
uncertainty [4]. The 243Am targets were irradiated in 1
MW power operation with the pneumatic tube Pn-2. The
bare target was irradiated for 30 min, and that with a Gd
filter for 5 min. Gamma rays emitted from irradiated Am
samples and alloy wires were measured with a high-purity
Ge detector.
Next, for the 243Am(n,J)244m+gAm reaction, the amountsof 244mAm and 244gAm produced via neutron capture reaction
were determined from the D-ray yield of their daughter nucleus 244Cm. The 243Am targets with and without a Gd shield
were irradiated for 6 hours by the hydraulic conveyer in 5
MW power operation. After irradiation, a cooling time for 5days caused 244gAm sufficiently to decay to 244Cm. At thistime, the amount of 244gAm was reduced to about 1/4000.
Irradiated fiber filters were rinsed with 3M HNO3 solution
and the solution was centrifuged. The separated supernatants
were dropped onto Petri dishes, and dried to make D-ray
samples. Alpha-ray measurements were done with the model
7401 alpha spectrometer (Canberra, Inc.).

$QDO\VLV Neutron fluxes at the irradiation positions wereobtained from the induced activities of the monitor wires.
)LJXUH  shows an example of J-ray spectrum due to the
decay J-rays emitted from 244gAm produced by the
243Am(n,J)244gAm reaction. Its measurement time was 16
hours. For the 243Am(n,J)244m+gAm reaction, )LJXUH 
shows an D-ray spectrum obtained by 168-hours measurement. Reaction rates of the 243Am were obtained fromamounts of the 243Am samples and produced nuclides. Theirreaction rates and neutron flux information were analyzed on
the basis of Westcott’s convention [5] to derive neutron capture cross sections. Data analysis is in progress.

)LJAn example ofJ-ray spectrum of irradiated 243Am sample.

)LJAn example ofD-ray spectrum of irradiated 243Am sample.

$FNQRZOHGJHPHQW
Present study includes the result of “Research and Development for accuracy improvement of neutron nuclear data on
minor actinides” entrusted to the Japan Atomic Energy Agency by the Ministry of Education, Culture, Sports, Science andTechnology of Japan (MEXT).
5HIHUHQFHV>@ http://www.nucleide.org/Laraweb/index.php>@ K.Okumura HWDO., JAERI-Research2004-025.
>@ R.W.Hoff HWDO., 3K\V5HY&. 1984 618.
>@ S.Nakamura HWDO., -1XFO6FL7HFKQRO.  2019123.
>@ C.H. Westcott HWDO., “3URFQG,QW&RQI3HDFHIXO
8VHRI$WRPLF(QHUJ\*HQHYD”,  1958 70.

31020

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4XDQWLWDWLRQRI*DPPD5D\(PLVVLRQIURP&DSXWUH5HDFWLRQRI8UDQLXP

Y. Nauchi, J. Hori1 and T. Sano2
1XFOHDU7HFKQRORJ\5HVHDUFK/DERUDWRU\&HQWUDO5H
VHDUFK,QVWLWXWHRI(OHFWULF3RZHU,QGXVWU\.\RWR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG
1XFOHDU6FLHQFH$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\,1752'8&7,21 For the criticality control and thesafeguards of fuel debris formed in the Fukushima
Dai-Ichi nuclear power station, quantification of the massof nuclear materials and its residual fissile enrichment isdesirable. However, non-destructive quantification techniques have never been developed even for intact spent
nuclear fuel assemblies. In the conventional fuels forlight water reactor utilization, the dominant nuclide of thefuel mass is 238U. Thus, we have focused on measurementof J rays from capture reactions of 238U by neutron induced J ray spectroscopy (NIGS). We have succeeded in
detection of 4060 keV J rays from capture reaction of238
U from a sub-critical core [1]. Furthermore, we foundthat the count rate ratios of the 4060 keV J ray to fission
prompt ones are consistent with 238U/235U ratios in two
sub-critical cores of different average 235U enrichments[2]. However, the J ray spectrum from the reaction has
been reported to vary with the incident neutron energy [3].
To utilize the NIGS spectrum for the quantification of thenuclear material and the enrichment, the J ray spectrum
measurement was conducted in this work.
(;3(5,0(176 The measurement was conducted in
LINAC pulsed neutron source facility in KURNS. A
tungsten (W) target was irradiated by accelerated electron
and the Bremsstrahlung photons were radiated. Then thephoton interacted with W and photo nuclear reactions
were induced. The beam frequency was adjusted to 50 Hz
and the pulse width was 1 Ps (nominally). The beam current was stabilized to 27 PA. The target was located on
center of a cylindrical tank of 20 cm in diameter and 30
cm in height. The tank was filled with light water. The
neurons generated in the W target was moderated in thewater. We used the neutron at “12 m room” which is located on 135 deg axis from the electron beam line. In theroom, a square shaped sample of metallic U was irradiated by the moderated neutron. Its geometry was 4 cm
4 cm and the thickness corresponds to 2.91 g/cm2. A
HP-Ge detector of 35% relative efficiency was set on 90
deg axis from the neutron flying axis. The distance fromthe center of the sample to the head of the detector was 5
cm. The detector was carefully shielded from the J - flashfrom the target. The J ray pulse height in the detector was
acquired together with the time of flight (TOF) information. The pulse height was calibrated with additional
measurement of 35Cl(n,J) reactions. The energy of theneutron inducing the 238U(n,J) reaction was deduced fromthe TOF information. TOF spectra was calibrated withadditional transmission measurements through Mn, In,

Ag, Cd. The effective length of the flight path was deduced to be 11.3m.
5(68/76 In figure 1, the J ray pulse height spectra are
given for several neutron energy regions: the thermal, theepi-thermal, and the resonances of 238U(n,J) reactions. In
the thermal and epi-thermal regions, 238U(n,J) J rays were
measured simultaneously with prompt and delayed ones
from fission reactions of 235U. For the resonance energies,
it is considered that the 238U(n,J) J rays are dominant. In
every region, 4060 keV J ray was detected. The energy
resolution of this experiment was better so that 3982 and3991 keV components are resolved, which has neverbeen done with 4S type HP-Ge detector [3]. 3583 and3197 keV J rays were measured especially for the En=
6.67 eV resonance. However, 3567, 3541 and 3482 keV J
rays [3] were not clearly resolved due to the counting
statistics and the single escape peaks. In CapGam [4],yield of 3296.5 keV J ray is evaluated larger than that of
4060 keV J ray for the thermal neuron capture of 238U.
However, the 3296.5 keV J ray peak was not found forreactions for every neuron energy region.
The J ray spectra were observed differently for incident
neutron energies. On account of the difference, ratio ofsome resonances to the thermal 238U(n,J) reaction might
be unfolded by spectra obtained by NIGS. Thus, NIGS
would be a new validation tool for neutron spectrum calculation in the reactor physics field, which has neverbeen achieved. For the purpose, 238U(n,J) J ray measurements with better statistical accuracy is further desired aswell as nuclear data evaluation.
㼠㼔㼑㼞㼙㼍㼘
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&2

㻟㻡㻤㻟

㻝㻜㻜㻜

㻝㻜㻜

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㻟㻞㻜㻜

㻟㻠㻜㻜 㻟㻢㻜㻜 㻟㻤㻜㻜 㻠㻜㻜㻜㻼㼡㼘㼟㼑㻌㼔㼑㼕㼓㼔㼠㻌㻔㼗㼑㼂㻕㻠㻞㻜㻜

Fig. 1 Measured pulse height spectrum for U sample.
5()(5(1&(6[1] Y. Nauchi, T. Sano, H. Unesaki, S. Sato, M. Suzuki, H.
Ohta. Proc. ICNC2019.
[2]Y. Nauchi, S.Sato, M. Suzuki et al., KURNS progress
report 2018, CO3-10.
[3] H. Harada, S.Goko, A.Kimura, et al, J. Korean Phys.
Society 59(2) 1547-1552, 2011.
[4] E. A. McCutchan manages, “Thermal Neutron Capture J’s by Target”, browse on Jan5, 2020.

31022
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&2'HYHORSPHQWRIFXUUHQWPRGHQHXWURQGHWHFWRUVIRU%1&7ILHOGV

T. Matsumoto, A. Masuda, H. Harano, J. HoriDQG T.Sano

clearly, although signals due to gamma flash from thetarget were successfully observed.

1DWLRQDO0HWURORJ\,QVWLWXWHRI-DSDQ1DWLRQDO,QVWL
WXWHRI$GYDQFHG,QGXVWULDO6FLHQFHDQG7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\,1752'8&7,21  Evaluation of neutron fluence andneutron dose equivalent for the epi-thermal neutron region is very important to manage workplaces with neutron sources or nuclear fuels as well as irradiation fields ina boron neutron capture therapy (BNCT). In the pre-sent
study, we have developed a current-mode neutron
detector [1] that can be used in intense neutron flux fieldsuch as BNCT fields. The neutron detector is composed ofa pair of 6Li-glass and 7Li-glass scintillators (10-mm
diameter and 2-mm thickness).
The current outputs
from photomultipliers are directly used to evaluate theneutron fluence in the detector. We have tried to apply
the current-mode detectors to sensors used in a neutron
detection device with a moderator. We fabricated four
pairss of the current-mode detector (four 6Li-glass and
The individual
four 7Li-glass scintillation detectors).
difference was evaluated to precisely measure neutrons
using the neutron detector device with the moderator.
Moreover, we fabricate a prototype of 6Li-glass scintillation detector with a photodiode (Fig. 1). We also experimentally verified the 6Li-glass scintillation detector
with the photodiodeFig. 1. Prototype of the 6Li-glass scintillation detector with the photodiode.

(;3(5,0(176 A collimated neutron beam with 30
mm diameter was obtained by the photo neutron reaction
using a tantalum target with a water moderator at the
KURRI Linac [2]. Figure 2 shows the experimental setup.
The detector was set at 12 m away from the target. An
enriched 10B4C sample with 10-mm thickness was also
used to subtract background thermal neutrons in themeasurement room. The 10B4C sample was set between
the detector and end of the collimator in the beam line. A
BF3 proportional counter was used as a neutron moni-tor.
All data were normalized using counts obtained with
Characteristics of thethe BF3 proportional counter.
neutron detection were experimentally evaluated bymeans of the time-of-flight (TOF) method.
5(68/76 Figure 3 shows the relative sensitivity of
the 6Li-glass and 7Li-glass scintillation detectors forthermal neutron region, respectively. The thermal neutron sensitivities for the 6Li-glass scintillation detectors
were agreed within 0.5 %. The sensitivities for the7
Li-glass scintillation detectors had variation within 6 %.
It is guessed that the neutron sensitivity of the 6Li-glass
scintillation detector with the photodiode is lower thanthat with the photomultiplier, because of difference ofphoton sensitivities of the photon detectors for 470 nm
photon from the 6Li-glass scintillator. In the first experiments of 2019, signals due to neutrons were not observed

Fig. 2. Experimental setup for the 6Li-glass scintillation detector. The detector was set at 12 m awayfrom the target.
10
Net counts/Monitor countNet counts/Monitor count

220

210

8
6
4
2
0

200
01

02
03
GS20-detector number

04

05

06
07
GS30-detector number

08

Fig. 3. Results of neutron sensitivities for the6
Li-glass (GS20) and 7Li-glass (GS30) scintillation
detector.
5()(5(1&(6>@ K. Kobayashi et al., Annu. Rep. Res. Reactorinst.
Kyoto Univ. 22, 142 (1989).
>@ T. Matsumoto et al., Radiat. Prot. Dosim. in press(https://doi.org/10.1093/rpd/ncz266)
This
work
was
supportedby
JSPS
KENHI(JP16K21679, JP16K09030, 19K12638).

31102

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KA-

&2

0HDVXUHPHQWVRIWKHUPDOQHXWURQWRWDODQGVFDWWHULQJFURVVVHFWLRQRIPRGHUDWRUPDWHULDOV-XQ1LVKL\DPD-DHKRQJ/HH7DGDIXPL6DQRDQG-XQLFKL+RUL/DERUDWRU\ IRU $GYDQFHG1XFOHDU (QHUJ\ ,QVWLWXWHRI,QQRYDWLYH5HVHDUFK7RN\R,QVWLWXWHRI 7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR 8QLYHUVLW\$&.12:/('*(0(176  This research is a collaborative effort of Toshiba Energy Systems & Solutions,Kindai University, Kyoto University and Tokyo Instituteof Technology.
5()(5(1&(6[1] R. Kimura and S. Wada, Nucl. Sci. Eng., Vol.193,
p.1013-1022, (2019).

$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\-DSDQ$WRPLF(QHUJ\$JHQF\ -XQHa 

,1752'8&7,21  The high temperature gas-cooled
reactor is a Generation IV reactor concept that use a graphite moderator. The design takes advantage of the inherent
safety characteristics with specific design optimizations.
The treatment of thermal scattering caused by crystalline
is important for graphite to improve the prediction accuracy of graphite moderated core analysis. There is sufficient thermal scattering law for single crystal graphite, butthere is no method has been established to reconstruct thermal scattering cross section for polycrystalline graphite.
On the other hand, a new concept of small modular reactor
using CaH2 as solid moderator has been developed [1]. The
experimental and evaluated data of the thermal scattering
law for CaH2 are insufficient. In order to provide basic data
for thermal neutron scattering law evaluation, the total andscattering cross sections of moderator materials were
measured.

Fig 1. Experimental arrangement
Table 1 &haracteristics of samplesSampleStructure(;3(5,0(176 The total and scattering cross sections of moderator materials were measured in the incident
neutron energy region from 0.001 to 10 eV by transmission
and scattering experiments at the KURNS-LINAC. An experimental arrangement is shown in Fig. 1. Pulsed neutrons were produced from a water-cooled Ta-target by (J,n)
reaction with a pulsed electron beam. The incident neutron
spectrum on a sample, the transmitted and scattering neutron spectrum were measured by means of a time-of-flight(TOF) method with a 6Li-glass scintillation detector. A 5.0
mm diameter by 5.0 mm thick 6Li-glass was located 12.0
m from the neutron source. The scattering neutrons were
measured by a 50 mm diameter by 5.0 mm thick 6Li-glass
scintillation detector. The scattering neutron spectra wereobserved at angle of 45 degrees with respect to the neutron
beam direction.
 The characteristics of the samples are shown in Table 1.
The graphite and polyethylene sample are used as a moderator in the KUCA facility.
5(68/76 The total cross sections of moderator materials were derived in the incident neutron energy region
from 0.001 to 10 eV. Figure shows the scattering neutron
specta.The result of graphite had a structure caused by themal scattering crystalline. Figure 3 shows the scattering
neutron spectrum with the resonance filter (Cd, In, Ag,
Mn). It was shown that it is possible to measure quasimonochromatic neutrons from a white neutron source.

Graphite
Polycrystalline

CaH2
PowderSample shape

Polyethylene
High molecular
Square plate

Square plate

Density [g/cm3]
Size [mm]Thickness [mm][atoms/b]

0.949
50.850.8
3.18
1.2610-2

1.754
50.850.8
12.7
1.1210-1

Disk in Al
case
1.200
I50
5.0
8.6310-3

Fig. 2 Scattering neutron energy spectra

Fig. 3 Scattering neutron energy spectrum with resonancefilter (Cd, In, Ag, Mn)

31108

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&2 0HDVXUHPHQWRI7HPSHUDWXUHGHSHQGHG7KHPDO1HXWURQ6SHFWUXPLQ6ROLG0RGHUDWRU
T. Sano, J. Lee1,3, J. Hori1, J. Nishiyama2$&.12:/('*(0(176This research is a collaborative effort of Toshiba Energy
Systems & Solutions, Kindai University, Tokyo Instituteof Technology and Kyoto University.

$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
/DERUDWRU\IRU$GYDQFHG1XFOHDU(QHUJ\7RN\R,QVWLWXUHRI7HFKQRORJ\-DSDQ$WRPLF(QHUJ\$JHQF\ -XQa ,1752'8&7,21In recent years, small modular reactors (SMR) havebeen studied intensively. Those SMR are employed existing technologies such as light-water moderator andcoolant and so on. On the other hand, a new concept of
SMR using solid moderator has been developed [1]. Here,the moderator in a nuclear reactor is common material
such as light-water, researchers and engineers could calculate the accurate neutron spectrum in the moderator byusing evaluate nuclear data libraries such as the
JENDL-4.0 [2]. However, if evaluate nuclear data libraries has poor data for moderator materials, the calculationsof accurate neutron spectrum in the moderator will bedifficult. The new concept of SMR is employed CaH2 assolid moderator [1].
Therefore, in order to perform a nuclear design for thereactor with CaH2, it is necessary to experimentally investigate the temperature-dependent neutron spectrum inthe moderator. In last year, a preliminary experiment of
temperature-dependent neutron spectrum measurements
was carried out [3]. In the present study, the experimental
geometry and condition were optimized based on the
results of preliminary experiment and the temperature-dependent neutron spectrum measurements were
performed.

5()(5(1&(6[1] R. Kimura and S. Wada, Nucl. Sci. Eng., Vol.193,
p.1013-1022, (2019).
>@ K. Shibata, et. al., J. Nucl. Sci. Technol., 39(11),(2002).
>@ J. Lee, et. al., Proc. on ND 2019, Beijing, China, May
19-24, (2019).

)LJ([SHULPHQWDOJHRPHWU\

7DEOH([SHULPHQWDOFRQGLWLRQ
6DPSOH

&D+
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WLPH K 

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
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7DEOH6DPSOHLQIRUPDWLRQ(;3(5,0(176To measure the temperature-dependent thermal neutron
spectrum in CaH2 sample, a preliminary experiment was
conducted method in KURNS-LINAC. The CaH2 sample
was set in a heater to be increased the sample temperaturefrom 21Υ to 470Υ. Figure 1 shows an experimental
geometry of present study. The heater was installed at a
positon of 12.6 m from the pulsed neutron source at
KURNS-LINAC. In this experiment, a GEM type neutron detector was employed. The neutron flight length
between the CaH2 and the GEM detector was 60 cm. Table 1 shows the experimental conditions and Table 2 isthe sample information. The transmitted neutron flux
from the sample was observed by the TOF method in thepresent study.
5(68/76
The obtained thermal neutron TOF spectrum of theCaH2 at room temperature (21Υ) and 470Υ are shownin the Fig. 1. The difference of thermal neutron spectrum
between 21Υ and 470Υ was clearly observed.

/,1$&
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35Hz, 3ȣs, 53ȣA
35Hz, 3ȣs, 53ȣA
35Hz, 3ȣs, 53ȣAChemical formulaDensity
Geometry

CaH2
1.33 g/cm3
70 mm  70 mm 60 mm)LJ 2EWDLQHG WKHUPDO QHXWURQ 72) VSHFWUXP RI
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31156

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%DVLF5HVHDUFKIRU6RSKLVWLFDWLRQRI+LJKSRZHU5HDFWRU1RLVH$QDO\VLV ,, 

S. Hohara1, T. Sano1, A. Sakon1, K. Nakajima2, K.
Takahashi2, K. Hashimoto1
$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\OQWHUGLVFLSOLQDU\*UDGXDWH6FKRRORI6FLHQFHDQG(Q
JLQHHULQJ.LQGDL8QLYHUVLW\
,1752'8&7,21  Reactor noise for high-power reactors were actively measured in the 1960’s and 1970’s.
The major focuses of those researches were for the abnormality diagnosis or the output stabilization diagnosis,
and almost researchers were in the field of system control
engineering or instrumentation engineering. High-powerreactor noise measurements for dynamics’ analysis ofreactivity change, reactivity feedback or reactor characteristics itself were few in the time (1960’s and 1970’s),
because of the powerless measurement system. In thisresearch, we plan to measure KUR’s output with present-day measurement system and plan to analyze withseveral analysis methods. The results of this work will
supply some knowledges and technics in the aspect ofsophistication of reactor noise analysis or simulation
methods.
In this year, we tried to measure the reactor nuclide noiseof the critical state KUR core via a 1-inch 3He counter at
CN-1 port. The experimental work was done in 7th November 2019. As the result of the experiment, a result
looks like the nuclear reactor noise was observed.
(;3(5,0(176 In this experiment, the output signalof the 3He counter was put into a Spectro Scopy AMP(2022: Canberra), and the output of the SSA was measured with a time-series measurement system (HSMCA4106_LC: ANSeeN Inc.). A schematic view of themeasurement is shown in Fig.1, and the counter installation overview is shown in Pic.1.

Fig. 2. An overview of the counter installation

No.
1
2
3
4

Table 1. Experimental condition
ReactorMeasurement
Count Rate
PowerTime [sec]
[cps]
[W]
20
800
0.54
100
600
2.73
300
1,000
7.92
1k
3,600
26.33

5(68/76
The measurement results were analyzed by Feynman-α /bunching method. As a result of the analysis, good results
were not obtained for 20W, 100W and 300W. However, aplot shape similar to Feynman's theoretical formula was
obtained for 1kW. The analysis result is shown in Fig.3.
From the result, the prompt neutron decay constant was
97.7 [sec-1], and y value was very small (~0.09). Fromthe smallness of the Y value, it is considered necessary toverify whether it is a nuclear noise by other techniques(e.g., covariance to mean ratio method, etc.).

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The experimental condition is shown in Table.1. The reactor Power was set from 20W to 1kW. The measurement
time was 800 ² 3,600 sec.

31025

‑137‑

Fig. 3. A Feynman- α/Bunching analysis result for the
1kW KUR operation

'HPRQVWUDWLRQ RI DGYDQFHG VXEFULWLFDO PHDVXUHPHQWV 7LPH'RPDLQ'HFRPSRVLWLRQEDVHG,QWHJUDO 7'', PHWKRGDQGWKLUGRUGHUQHXWURQFRUUHODWLRQWHFKQLTXH

T. Endo1, K. Watanabe1, A. Nonaka1, S. Imai1, F.
Nishioka1, H. Oike1, M. Yamanaka2, C.H. Pyeon2
*UDGXDWH6FKRRORI(QJLQHHULQJ1DJR\D8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In a general transient in a subcritical system, reactivity, neutron source intensity 6, andpoint kinetic parameters (Λ and ȕeff) can change simultaneously. For such a simultaneous transient, the subcriticality measurement by the conventional neutron source
multiplication method or inverse kinetics method is difficult because 6 and point kinetics parameters are generally assumed to be constant. To address this issue, wedeveloped the time-domain decomposition-based integral(TDDI) method [1] to measure the subcriticality in dollar
units after the transient. Furthermore, for an unknown
target system with a steady-state, it is not easy to estimate
an absolute value of subcriticality, íȡ, without additional
information such as detector efficiency, source strength,
and preliminary numerical analysis. To roughly estimate±ȡ in the stationary unknown system, we have been investigating the third-order neutron correlation  technique [2], which is a zero-power reactor noise analysis
method using the second- and third-order factorial moments of neutron counts. In this study, advanced subcritical measurements using the TDDI method andthird-order neutron correlation technique were conductedto confirm these applicability in subcritical cores at the
Kyoto University Critical Assembly (KUCA). This reportmainly presents experimental results using the TDDI
method.
0(7+2'2/2*<  The TDDI method was proposedusing the point kinetics theory based on the fundamental
mode approximation. This method assumes that a target
subcritical system changes from a steady-state into another steady-state via an arbitrary transient of statechange (HJ subcriticality, source strength, and point kinetics parameters) during W0WW1. Using the measured
time variation in neutron count rate Q(W)under such a situation, an absolute value of subcriticality in dollar units
after the transient (íȡ1ȕeff,1) can be evaluated by the followingg formula:method [1] with the assumption where the probability
distribution of neutron counts approximately follows the
Poisson distribution.
(;3(5,0(176  The subcritical transient experiments were carried out in a deep subcritical core(A(1/8”p60EUEU(3)+1/8”p10EUEU<EUEU-AlAl-NUAlAl-EUEU>)) driven by a spallation neutron source,which was generated by colliding a 100MeV proton
beam from the FFAG accelerator with a Pb-Bi target. All
control and safety rods were fully inserted. Time series
data of neutron count rate, Q(W), was continuously measured using neutron detectors (LiFCaF and LiF/Eu:CaF2
fiber-type detectors (#1,4) in the core region and BF3counters (#1,3,4) in the polyethylene reflector region)
with list-mode data acquisition systems. First, the subcritical core was kept under the steady-state driven by thespallation source to obtain the stationary count rate Q0
before the transient. Second, a ramp-wise transient wasgiven by withdrawing 3×3 fuel and reflector assemblies
in approximately 15 seconds. Thereby, not only the subcriticality but also point kinetics parameters simultaneously changed over the withdrawing time. After the transient, the core was kept as-is for a sufficiently long time
until the subcritical core reached another steady-state tomeasure stationary count rate Q∞ after the transient. Basedon Eq. (1), íȡ1ȕeff,1 was estimated from the measured
Q(W). For comparison, the subcriticality using the conventional integral method was also estimated.
5(68/76 Figure 1 shows experimental results ofíȡ1ȕeff,1 by the conventional integral and TDDI methods
for five neutron detectors, and the numerical result by
MCNP6.2 with ENDF/B-VII.1 (10.20±0.08 [$]). In thecase of the conventional integral method, íȡ1ȕeff,1 values
were significantly underestimated compared with the
MCNP6.2 result, and these differences were larger than
the statistical errors. On the other hand, íȡ1ȕeff,1 of the
TDDI method well agreed with the MCNP6.2 result.
Consequently, the applicability of the TDDI method wasdemonstrated through this KUCA subcritical transient.
15
MCNP6.2,
ENDF/B-VII.1

TDDI method

10

[$]

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5

3

4

5

BF3#4

2

BF3#3

1

BF3#1

0

Fiber#4

conventional integral method0Fiber#1(1)
where Q0 and Q∞ means the stationary neutron count rates
before and after the transient; DL and ȜL represent relative
delayed neutron yields and decay constant for Lth precursor group. The TDDI method has advantages to approximately estimate the subcriticality without the following
information: (1) the reference subcriticality íȡ0 before
the transient, (2) the absolute values of neutron source
intensity and the point kinetics parameters before andafter the transient, and (3) the time variation in them. The
statistical error of íȡ1ȕeff,1 using the TDDI method canbe approximately estimated using the random sampling

6

Figure 1. Experimental results of TDDI method.
5()(5(1&(6[1] T. Endo, HW DO, J. Nucl. Sci. Technol., (2019).
DOI:10.1080/00223131.2019.1706658[2] T. Endo, HW DO, J. Nucl. Sci. Technol.,  (2019)322–336.

CA3101‑138‑

Measurement of Gamma Ray from Short Lived Fission Product underBackground of Fission Prompt Gamma Ray)LJ([SHULPHQWDOVHWXS
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&$

‑139‑

&2

5HDFWRU1RLVH3RZHU6SHFWUDO$QDO\VLVIRUD*UDSKLWH0RGHUDWHGDQG
5HIOHFWHG&RUH ,,A. Sakon, K. Hashimoto, S. Hohara, K. Nakajima1,
K. Takahashi1, T. Sano1, Y. Fukaya2, N. Fujimoto3, and Y.
Takahashi4.LQGDL8QLYHUVLW\$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH*UDGXDWH6FKRRORI6FLHQFHDQG(QJLQHHULQJ.LQGDL8QLYHUVLW\
6HFWRURI)DVW5HDFWRUDQG$GYDQFHG5HDFWRU5HVHDUFK
DQG'HYHORSPHQW-DSDQ$WRPLF(QHUJ\$JHQF\)DFWXOW\RI(QJLQHHULQJ.\XVKX8QLYHUVLW\ 
,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 In the last study, the prompt neutron
decay constants measured by the detectors about 30cm
and 35cm away from core region agreed with the calculated results by the continuous-energy Monte Carlo code
MVP version 3[1]. The location of these detectors is farther than the location in the light water moderation reactor. The objective of this study is experimentally to confirm a high flexibility of neutron detector placement ingraphite reflector for reactor noise analysis.

Reactor noise analysis by power spectrum method was
performed in the critical state of suitable reactor power
for each detector. The reactor power during measurement
was adjusted so that the count rate of each detector was
about 3,000[cps].
5(68/76 The auto power spectral densities by detector ”2” and detector “3” are shown in Fig. 2 and Fog. 3,
respectively. These figures also include least-squares fitsof a conventional formula [2] to the spectral densities todetermine the prompt-neutron decay constant D0 (Eeff//),where the fitting was confined to a frequency range from1.25 to 100 Hz. The derived decay constant of detector“2” was 65.8±3.4[1/s], which was about the same as thatthe graphite core of last year. However, the derived decay
constant of detector “3” was 96.3±14.3[1/s]. in order toobtain the prompt-neutron decay constant using a detector more than 35cm away from core regions, it is necessary to efficiently measure neutrons that information on
fission reaction.
Graphite core Ver. 2019, Pattern S-2 (Critical)

0

-3 10

(;3(5,0(176 The core configuration is shown in
Fig. 1. “F” denoted a low-enriched fuel assembly, whose
average enrichment is 5.41wt%. “D” is a driver highly-enriched fuel assembly. “G” is graphite reflector. Orange cell is polyethylene reflector. “1”, “2”, “3”, andblack dots are BF3 proportional neutron counters. Withedot is 3H proportional neutron counter. These counters are
1.0 in. diameter and 15.47 in. length. In a critical state,
reactor noise analysis was carried out using BF3 detector“1”, “2”, and “3”. The distance from core region to detector “1” is about 20cm, that to detector “2” is about
35cm, that to detector “3” is about 55cm.

0

APSD

2

-1

-4 10

D0 =65.8㼼3.4[s ]0(2.5~100Hz)

-5 10

2
0

䃅㻌[V2] -6 10

0

-7 10

0

-8 10

1

10
Frequency[Hz]100Fig. 2 Auto-Power Spectral Density (Detector “2”)0

-5.5 10Graphite core Ver. 2019, Pattern S-3 (Critical)
3

0

-6 10
APSD

3

-1

D0 =96.3㼼14.3[s ](2.5~100Hz)0-6.5 10
䃅㻌[V2]

0

-7 10

0

-7.5 10 1

10Frequency[Hz]100Fig. 3 Auto-Power Spectral Density (Detector “3”)
5()(5(1&(6Fig. 1 Core configuration(B7/4”G2/8”p8EUNU+3/8”p38EU)[1] Y. Nagaya, K. Okumura, T. Sakurai and T. Mori,
MVP/GMVP Version 3 : General Purpose Monte Carlo
Codes for Neutron and Photon Transport Calculations
Based on Continuous Energy and Multigroup Methods,
Tokai-mura: Japan Atomic Energy Agency; 2017,(JAEA-Data/Code 2016-018).
[2] M. M. R. Williams, Random Processes in Nuclear
Reactors, (Pergamon Press, Oxford,1974), section 3.6.

CA3104‑140‑

&2

Measurement of fundamental characteristics of nuclear reactor at KUCA (IV)< .LWDPXUD70LVDZD06]LHEHUWKDQG*.OXMEHU
1Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Institute of Nuclear Techniques, Budapest University ofTechnology and Economics
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Channel1
Channel2
Channel3
Channel44

3.5
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,1752'8&7,21  To introduce noise analysis technique to High Temperature engineering Test Reactor(HTTR), noise measurement is performed based on
B7/4”G2/8”p8EUNU+3/8”p38EU(3) core composed in
the B-rack of Kyoto University Critical Assembly (KUCA). In the previous experiment performed last year, theneutron source was set to out of core. In the present experiment, the neutron source of Cf was loaded into a fuelassembly(;3(5,0(176 The core configuration is shown in
Fig.1. First, the fuel assembly with neutron source was
loaded into the center of the core at T15 to mimic thepower distribution in criticality. Second, that wasloaded into the edge of the core at G15 to mimic thepower dis-tribution of the HTTR in subcriticality andneutron leak-age directly to the neutron detectors. In thiscase, the BF3 detector was moved from I15 to O21. In
this report, the first case is called “criticality mimickedcase”, and the second case is called “HTTR mimickedcase”. The reac-tor noise driven by inherent neutron
source was alsomeasured and is called “inherent neutron source case.”
For these data, we apply Feynman-α method to observesub-criticality. The control rods pattern and subcriticality
is listed in Table 1
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Fig. 1 Core configuration
Table 1 Control rods pattern and subcriticality㻯㼛㼚㼠㼞㼛㼘㻌㻾㼛㼐㻌㻼㼛㼟㼕㼠㼕㼛㼚㻌

ChannelDecay constant (s-1)

C

Ch.3

167.8±0.91.250±0.011

D

Ch.3

239.4±1.82.105±0.021

E

Ch.3

343.6±4.93.349±0.059

Subcriticality (-%Δk/k)

Table 3 Decay constant and subcriticality of criticality
mimicked case

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Table 2 Decay constant and subcriticality of inherent
neutron source case

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5(68/76 To determine the prompt neutron decay constant, Feynman-Y is evaluated and the curve is fitted toan analytical formula by non-linear least square method
as shown in Fig. 2. In general, the plotted Feynman-Y
shows a good agreement with the analytical formula. The
results are summarized in Tables 2, 3 and 4, respectively
for the inherent neutron source case, criticality mimicked
case, and HTTR mimicked case. Here, we focus on Ch.3
to observe directly detected neutron effect.
Comparing those result, the characteristics is found as
follows:
࣭Generally, the inherent neutron source cases show agood agreement with the subcriticality measured byrod drop method listed in Table 1 without dependingon the subcriticality. It is supposed that the neutron
source distributes similar to the power distribution in
criticality.
࣭With the external neutron source cases, WKDWLV criticality
mimicked case and HTTR mimicked case, the subcriticality shows slight different with the shallow subcriticality control rod pattern.
࣭In the HTTR mimicked case, the difference is slightly
larger than that in the criticality mimicked case. It is
guessed that the error is caused by the directly detected
neutron from the neutron source.

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Ch.3

183.2±1.11.434±0.013

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Ch.3

215.2±2.31.816±0.027

E

Ch.3

381.5±7.73.801±0.424

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Center

Subcriticality

C1

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[- %Δk/k]

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0.857

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191.8±2.01.537±0.023

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254.7±2.92.288±0.034

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3.715±0.116

Pattern

Table 4 Decay constant and subcriticality of HTTR mimicked case

CA3107‑㻝㻠㻞‑

Subcriticality (-%Δk/k)

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M. Fukushima1, A. Oizumi1, M. Yamanaka2 andC. H. Pyeon2


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,QVWLWXWHIRULQWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The Japan Atomic Energy Agency(JAEA) has investigated neutronics of the accelerator-driven system (ADS) of a lead bismuth eutectic(LBE) cooled-tank-type core to transmute minor actinides discharged from nuclear power plants. For the design study of ADS, integral experimental data of nuclear
characteristics of LBE is necessary to validate cross sections of lead (Pb) and bismuth (Bi). Previously, Pb and Bi
samples experiments were performed in a high-enricheduranium (HEU) core [1]. In present study, a similar experiment was conducted in a variation of uranium corewith a low-enriched uranium region. (;3(5,0(176  The reference configuration had
five test rods as shown in )LJXUH. )LJXUH shows eachtest unit composed of two EU plates (1/16 inch×2), two
Al plates (1/16 inch×2), a natural uranium plate (1.05mm), two Al plates and two EU plates.The unit-averaged235
U enrichment was about 17%. The test units were axially and radially surrounded by normal fuel units composed of two EU plates and a polyethylene plate.
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In the previous experiments for sample worth, solid Al
plates were replaced with Pb (or Bi) plates, so aluminumcross sections should be considered as well as lead one(or bismuth) when verifying them. Instead, we used Al
voided spacers with a low density that was about 1/10
that of solid Al plates to reduce the aluminum component.
For the Pb sample worth, Pb plates instead of Al ones(See Figure 2) were installed in five test rods beforehand,and after then the Pb plates in the central 10 units were
replaced with Al voided spacers. The Pb sample worth
was estimated as difference excess reactivities before andafter the replacement. The other patterns were summarized together with experimental results in 7DEOH.
7DEOH Experimental results
Case

Pattern(U/&/B) *1

A
B
C
D
E
F

Pb/ 3E /Pb
Pb/ 9*2/Pb
Bi/ %L/Bi
Bi/ 9*2/Bi
Al/ $O*3/Al
Al/ 9*2/Al*1*2

Excess reactivity(pcm)
280.3 ± 6.5
116.1 ± 2.1
228.8 ± 6.6
75.6 ± 0.9
152.4 ± 5.6
33.0 ± 5.6

Sample worth(pcm)
Pb sample (A㸫B)
164.2 ± 6.9
Bi sample (C㸫D)
153.2 ± 6.7
Al sample (E㸫F)
119.4 ± 8.0(Upper 5 units / &HQWUDOXQLWV / Lower 5 units) of test regions.
9 indicates Al voided spacer. *3 $O indicates solid Al plate.

5(68/76 Numerical analyses were preliminary conducted with MCNP6.1 together with JENDL-4.0 (J40)
and ENDF/B-VII.1 (B71). The sample worth was estimated as the difference of the effective multiplication
factors between the sample-loaded and reference configurations, without considering the criticality bias. )LJXUH
shows that the calculations agree with experiment for the
Bi and Al sample worth. On the other hand, the calculations overestimate for the Pb sample worth. In FY 2020,
the re-measurement is planned also in HEU core by thesame method using Al voided spacers.

6& 6DIHW\RUFRQWUROURGV)LJXUH Reference configuration
Test units
20 times (275.00mm)
CentralLower
5 units
10 units

1/8"poly
1" Al(3.18mm)plate
1/16" Alʹ22.0"Graphite(50.80mm)(3.18mm)ʞUpper
5 unitsʞNU (1.05mm)

ʞ

11th unitʞ

6th unit

Polyethylene(469.9mm)

10 times(63.50mm)

1st unit

1/16" EUʹ2
(3.18mm)

10 times(63.50mm)

ʞPolyethylene(514.35mm)

2.0"Graphite(50.80mm))LJXUH Schematic drawing of test fuel rod

)LJXUH Results of sample worth
5()(5(1&(6[1] C. H. Pyeon, HW DO, J. Nucl. Sci. Technol., ,
602-612 (2016) and , 1324-1335 (2018)

CA3109‑143‑

&2

6XEFULWLFDOLW\PHDVXUHPHQWE\XVLQJDVPDOOQHXWURQGHWHFWRU

T. Misawa1, Y. Kitamura1, T. Takahashi1 and A. Yasui2

Rossi-alpha method.

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Ά * * * * * * * * * * * * * * * * * * * * * * * * * * * * *΃ * * * * * * * * * * * * * * * * 9ͳ 9,1752'8&7,21 Subcriticality monitoring system
has to be used to detect criticality approach for each stepof debris removal in Fukushima Daiichi nuclear power
plant. For this purpose, International Research Institutefor nuclear Decommissioning (IRID) is developing criticality control techniques for fuel debris removal based on
neutron noise analysis using Feynman-alpha method. A
prototype of the sub-criticality monitoring system wastested to verify applicability on various sub-criticality
measurement conditions.
For this measurement, a small neutron detector based on
a SiC with boron coated film is one of the candidates at
Fukushima because of its toughness against radiation
exposure and low detection efficiency for gamma-ray. We
are also developing a data transfer system from this SiC
neutron detector to data acquisition system which isplaced at outside of a reactor vessel by a specially designed optical fiber with high resistance against radiation.
In this research, we used this new data transfer system
which will be connected to a small neutron detector tomeasure subcriticality.
(;3(5,0(176Experiment was carried out at
KUCA solid moderated core, B-core, as shown in Fig.1
whose main fuel assembly was 2/8”p23EUEU with relatively hard neutron spectrum. This core was aimed tosimulate widely spread fuel debri. The fuel coupon plates
were sandwiched with polyethylene plates and assemblies were surrounded by polyethylene reflector to simulate water and some part of the core was assembled withgraphite region to simulate less water region which might
be appeared during fuel debri digging process. This core
was in subcritical state whose k-eff was approximately
0.89 and in steady state with Cf-252 neutron source inserted in a fuel assembly. Data transfer system is illustrated in Fig.2. Boron-lined neutron detector was inserted
in aperiphery fuel region whose neutron detection analog
signal was transfer pre-amplifier and then a data sendersystem by a co-axial cable. In the data sender system,
analog signal was changed to optical digital signal and it
was transferred to the data receiver system located at outside of the reactor room by a thin and long quartz opticalfiber cable. Then digital data was changed to analog datain the data receiver system and finally neutron detection
time whose time bin was 1 micro-second was transferred
to PC by USB cable and stored in PC.
'$7$ $1$/<6,6 Neutron detection time stamp datastored in PC wereanalyzed by the neutron noise analysis
methods, Feynman-alpha method (shown in Fig.3) and

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Fig.2 Data transfer system

Fig.3 Example of Feynman-alpha result5(68/76 As shown in Fig. 3, Y-values can be fitted
by the theoretical formula (red line) and prompt neutron
decay constant (alpha value) can be obtained by the leastsquare fitting method. By Feynman-alpha and Rossi-alpha methods, alpha value was 1110+/- 44 (1/s) and
1250+/-24 (1/s), respectively, and we are now comparing
those results with calculated ones by a computer code.
We are planning to use this data transfer system combined with a SiC neutron detector next year.

CA3110‑144‑

&2

9HULILFDWLRQRIDQLPSURYHGPHWKRGWRHVWLPDWHUHDFWLYLW\Y. Yamane, S. Araki, Y. Kitamura1, T. Misawa1-DSDQ$WRPLF(QHUJ\$JHQF\
,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The estimation of reactivity of anamount of unknown fissile material is one of important
issues in the field of criticality safety.
JAEA has been theoretically developing a method to estimate the reactivity and composition of fissile isotope
from neutron count rate alone[1-2]. The method is basedon a newly developed equation of power in quasi-steadystate after prompt jump/drop of power due to reactivity
and/or neutron source change[3].
The purpose of the experiment is to obtain the experimental data for the verification and validation of the developed method. This time, a fixed intensity neutron
source was used under shallow subcritical conditions, andan improved method which utilize the equation of power
as it is, not its integral, was applied to the measured neutron count rate data.
(;3(5,0(176 A subcritical core was made byremoving fuel elements from the basic critical core configuration known as 3/8’’ p36EU of A-core. The Am-Be
was used as the external neutron source.
3
He detectors were used. Figure 1 shows the core configuration and the position of Am-Be.
For the first several hundred seconds, as shown in Fig.2,
the system was kept under steady state. Then the removing of Am-Be started. It takes several minutes but an airduct was used to rapidly terminate the effect of neutron
injection to the core from Am-Be. After that, neutron
count rate decreased and the measurement terminatedafter one or several thousand seconds. Another measurement was done under steady state for several thousand
seconds in order to take data for Feynman-D method.

Fig. 2. Neutron count rate data. Blue circle shows
neutron counts per 0.01s and orange line shows a
profile of averaged neutron counts. Yellow line
shows a reproduced count rate.
5(68/76 A preliminarily estimated value obtainedby applying the new method to the neutron count rate
data was plotted against data by Feynman-D method in
Fig. 3, and the range of C/E was between 0.8 and 1.8.
The reason for large difference may be that the neutronfrom slowly moving Am-Be kept the power of the corehigh for a while after the start of removing and changed
the profile of neutron count rate from one without such
effect. It is expected that more detailed analysis will
make the reason clear.

Fig 3. The reactivity estimated by applying new
and neutron multiplication methods are plottedagainst that by Feynman-D method.

Fig. 1.
A-core.

Configuration of fuels and devices in

5()(5(1&(6[1] Y. Yamane, Proc. 2017 AESJ Spring meeting, 1F04,(2017) [in Japanese].
[2] Y. Yamane, S. Araki, Y. Kitamura, T. Misawa, Proc.
2019 AESJ Spring meeting, 2J02,(2019) [in Japanese].
[3] Y. Yamane, J. Nucl. Sci. Technol.
https://doi.org/10.1080/00223131.2020.1736682 (2020).

CA3111‑145‑

&2

Measurement of fundamental characteristics of nuclear reactor at KUCA (V)ZHUHUHDGE\DSUHDPSOLILHUDQGWKHQIHGLQWRWKHWUDQVPLWWLQJGHYLFH7KHVHVLJQDOV ZHUHWUDQVPLWWHGWRWKHUHFHLYLQJGHYLFHWKURXJKWKHRSWLFDOILEHU7KHWLPHVWDPSGDWDZHUHUHFRUGHGE\D3&< .LWDPXUD70LVDZD;;LDRDQG<+D\DVKL1Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2

Department of Fundamental Energy Science, Graduate
School of Energy Science, Kyoto University

3

Toshiba Energy Systems & Solutions Corporation

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T. Sano, K. Nakajima1, J. Hori2, Y. Takahashi2, H. Yashima2, and H. Unesaki2$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\

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41 unit cells

Driver fuel elemnt

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50 unit cells,1752'8&7,21In order to perform integral evaluation of the 232Th capture cross section, critical experiments with Th loaded various cores at KUCA has been
carried out [1]. In those critical cores, the H/235U nuclide
ratio were about 70 to 315 and the 232Th/235U nuclide
ratio were about 12.7 to 19.0. In this study, from theviewpoint of expanding critical experimental data, a newexperiment was conducted by a Th fuel loaded core with
51 of H/235U and 19.0 of 232Th/235U ratio at KUCA.
(;3(5,0(176 The new critical core consisted of twotype fuel elements. One was Th loaded fuel element, andthe other was driver fuel element shown in figure 1. A
unit cell of Th loaded fuel element had 2 enriched uranium (EU) plates with 1/16” thickness, 1 Th plate with
1/8” thickness and 1 polyethylene plates with 1/8” thickness. The Th loaded fuel element consisted of 27 unit
cells. A unit cell of driver fuel elements consisted of the 1
EU plate and the 2 polyethylene plates. The driver fuelelement had of 49 unit cells.
Figure 2 shows the core configuration of the critical experiment. There were the 37 Th loaded fuel elements (F)and the 32 driver fuel elements (D). Table 1 shows thecritical data of the core.
5(68/76 First of experiments, the neutronics characteristics of the Th loaded core was measured to check on
the parameters are fallen within the KUCA regulations.
Table 2 shows the measured neutronics characteristics.
The all characteristics are satisfied with the KUCA regulations.
In order to observe an effective multiplication factor(NHII) of the core, the excess reactivity worth was measured by the positive reactor period method. As the seven-times-measured results, the evaluated excess reactivity
worth was 0.0826s0.0034 (%dk/k) and the NHII was
1.00083s0.00003 [2]. The calculated NHII by MVP3.0[3]
with JELDL-4.0[4] was 1.00488s0.00002 and C/E value
was 1.0040 shown in 7able .
$&.12:/(*(0(17 A part of the present study was supported by CHUBU
Electric Power Co., Inc.
5()(5(1&(6>@ T. Sano et. al., Proc on PHYSOR2020, Cambridge,
UK, Mar.29th – April 2nd, (2020).
>@ T. Sano et. al., Abstract of AESJ Spring meeting,)LJ&RQILJXUDWLRQRIIXHOHOHPHQW

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Run No.
9855-1
No. of loaded EU plates
4634
No. of loaded Th plates
1517
Control Rod C1
723.14
position
C2
1201.14(mm)
C31201.37
S4, S5, S6
1200
14.9
Core temperature (Υ)
7DEOH0HDVXUHGQHXWURQLFVFKDUDFWHULVWLFVRIWKH7K
ORDGHGFRUH
Neutronics Charac- Measured
KUCA Regulateristics(%dk/k)tion
Excessreactivity
0.082< 0.35( %dk/k)(%dk/k)Rod worth C1 rod
0.319
Max. worth : <(%dk/k)1/3 of total
C2 rod0.397
worth
C3 rod0.390
Total*(0.319+0.397+ >Excess reactivity+
10.390)*2=2.212(%dk/k)Center core worth
2.329>1 (%dk/k)(%k/k)*S4, S5 and S6 rod worth are assumed same value as C1,C2 and C3 rods by symmetric geometry.

1I08, (2020).
>@ Y. Nagaya et. al., JAERI1348, JAEA, (2005).
>@ K. Shibata et. al., J. Nucl. Sci. Technol., 39(11),(2002)

CA3113‑147‑

7DEOH0HDVXUHGDQGFDOFXODWHGkeffMeasured
1.00083s0.00003
Calculated
1.00488s0.00002
C/E
1.0040s0.003 (%)

&2

&KDUDFWHUL]DWLRQRI$GGLWLYHLQ/XEULFDQWXVLQJ6PDOO$QJOH;UD\6FDWWHULQJY. Oba, M. Hino1, R. Motokawa, N. Adachi2, Y. Todaka2,
R. Inoue1, and M. Sugiyama1

-1

10 9
8
7

0DWHULDOV6FLHQFHV5HVHDUFK&HQWHU-DSDQ$WRPLF(Q
HUJ\$JHQF\
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6FKRRORI(QJLQHHULQJ7R\RKDVKL8QLYHUVLW\RI7HFKQOR
J\,1752'8&7,21  Lubricants usually contain a variety of additives to improve lubrication properties. In the
lubricants, the additives form nanostructures such as micelles, which play a key role in lubrication properties.
Small-angle scattering (SAS) is useful to characterizesuch nanostructures in solvent. However, SAS has been
scarcely used in the field of tribology [1].
Therefore, we performed small-angle X-ray scattering(SAXS) measurements of the additives in the lubricants
to determine proper experimental conditions and to obtain fundamental information needed for nanostructural
analysis.
(;3(5,0(176 SAXS measurements were performed using the in-house SAXS instrument with Mo .α
radiation. Scattering patterns were obtained using a
two-dimensional detector (PILATUS 100k) equippedwith a 1000 µm-thick silicon sensor. The path of X-ray
between the entrance slit and up to the detector including
the sample area was in vacuum to eliminate backgroundscattering from air and vacuum windows. Oleic acid
(OA) and oleyl acid phosphate (OLAP) were chosen as
the additives. 1 mass% oleyl acid phosphate and 5 mass%
oleic acid were dispersed in poly-α-olefin (PAO), respectively. The samples were sealed in sample cells made bystainless steel body, X-ray windows of cover glasses, andViton O-rings. Two samples-to-detector distances (SDD),
0.4 and 1.8 m, were used to cover wide T range, where T
is the magnitude of the scattering vector. The measurement times are 1 hour and 5 hours for 0.4 m and 1.8 m
conditions, respectively.
5(68/76 Fig. 1 shows the SAXS profiles of 5
mass% OA in PAO, 1 mass% OLAP in PAO, and pure
PAO. The scattering of an empty cell was subtracted as
background. A peak is observed at around T = 4.5 nm-1 inall the samples including pure PAO. This reflects thenanostructure in pure PAO. The profiles of the 5 mass%
OA in PAO are almost similar to those of pure PAO.

Intensity (arb. unit)

6
5
4
3

2

10

1% oleyl acid phosphate
5% oleic acid
PAO

-2

10

-1

10

0

10

1

-1

q (nm )

Fig. 1. SAXS profiles of 5 mass% OA in PAO, 1
mass% OLAP in PAO, and pure PAO. Open andfilled symbols indicate the profiles obtained using
SDD = 1.8 and 0.4 m, respectively.
Therefore, the scattering contrast of OA in PAO is probably too small to analyze. In contrast, 1 mass% OLAP in
PAO shows a significant increase in the scattering intensity at T lower than about 2.5 nm-1. This increase is thescattering of OLAP. The features of the scattering profiles
are similar to the scattering profiles of tri-Q-butyl phosphate in organic solvent [2]. This suggests that OLAP
forms aggregate in PAO. In summary, we successfully
observed the nanostructure of OLAP in PAO. For OA in
PAO, denser sample is required to obtain reasonable
scattering intensity.
$&.12:/('*0(176 A part of this work was
supported by JST "Collaborative Research Based on Industrial Demand" Grand Number JPMJSK1511, Japan.
5()(5(1&(6[1] M. J. Covitch HW DO, Adv. Chem. Eng. Sci.,  (2015)
134-151.
[2] R. Motokawa HW DO, J. Phys. Chem. B,  (2012)1319-1327.

31002

‑148‑

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Synthesis of alloy nanoparticles in water solution by two steps reduction
and one time γ-ray irradiation

F. Hori, Y.Uchimura, T.Yamada1, T.Matsui1, N.Taguchi2,
S. Tanaka2 and Q.Xu3
Dept. of Engineering, Osaka Prefecture University
1
Center for Advanced Education of Entrepreneurship andInnovation, Osaka Prefecture University
2
AIST, Kansai Center
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&2

Defects structure and characterization of electron irradiated intermetallic alloys

F. Hori, N.Ogawa, A.Takano, K.Sugita, T.Yamada,K. Ohsawa1, Q.Xu2 and N.Abe2*9&20)'/+.1-#/4'&#--093#.1-'3#//'#-+/)5140 
7+4**'#4+/)2#4'0( 3'% 

Dept. of Quantum & Radiation Eng., Osaka Pref. Univ.

5(68/76+)52' 3*0734*'!31'%42#0("25-
#--09 $'(02' +22#&+#4+0/ #(4'2 '-'%420/ +22#&+#4+0/ #/&
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1
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Res. Inst. of Appl. Mech., Kyushu University.8516

INTRODUCTION: / )'/'2#- +4 +3 7'-- ,/07/ 4*#4
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31'%4203%019  .'#352'.'/4 *#6' &0/' (02Fig. 2 TDS spectra of hydrogen desorption behavior forhydrogen charged ZrCuAl alloys with and without electron
irradiation.

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&2 0DJQHWLF6FDWWHULQJ&RQWULEXWLRQLQ,URQ&KDUDFWHU]HGE\1HXWURQ'LIIUDFWLRQY. Oba, K. Mori1, M. Hino1 and R. Okumura1
0DWHULDOV6FLHQFHV5HVHDUFK&HQWHU-DSDQ$WRPLF(Q
HUJ\$JHQF\
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Magnetic scattering contribution is
one of the most unique features of neutron diffraction andthus widely used for the investigation of magnetic structures. However, it is scarcely used in the research and development of practical ferromagnetic materials, such aspermanent magnets and soft magnetic materials. Since themagnetic scattering analysis can provide the information
about the directions of magnetic moments, it would be useful to understand magnetization process, which is a key toachieve higher permeability in the soft magnetic materials[1]. Therefore, we carried out the neutron diffraction experiments of the soft magnetic materials to confirm thatthe magnetic scattering contribution can be observed in themagnetization process.
(;3(5,0(176 An iron rod (99.9%) with the diameter of 12.7 mm was selected as a typical soft magnetic
material. The neutron diffraction experiments were performed using the Versatile compact neutron diffractometer(VCND) at the B-3 beam port of the Kyoto University Research Reactor (KUR) [2,3]. An electromagnet was placedon a sample goniometer to apply a magnetic field to thesample (Fig. 1). The maximum field is about 300 Oe.5(68/76 Fig. 2 shows the diffraction patterns of theiron rod and background. The iron rod shows clear Bragg
peaks at 31º and 44º corresponding to (110) and (200)planes, respectively. Small peaks at 29º, 42º, and 50º comefrom the background caused by the electromagnet.
The diffraction pattern with a magnetic field is also
shown in Fig. 2. The magnetic field was applied perpen-

Fig. 1. Photograph of electromagnet installed at
VCND. A magnetic field is vertically applied.
dicular to the scattering vector. In this condition, the magnetic scattering contribution must increase compared to ademagnetized state. The results indicate that the diffraction intensity with a magnetic field is higher than that without a magnetic field at the Bragg peaks, whereas the background intensity is not changed. This confirms that themagnetic scattering contribution can be observed in iron.
5()(5(1&(6[1] M. Birsan HWDO, Phys. Rev. B, (1996) 6412-6417.
[2] K. Mori HWDO, KURNS Prog. Rep. 2018, (2019) 128.
[3] K. Mori HWDO, JPS Conf. Ser., (submitted).

2

5

Intensity (10 counts)

3

with magnetic field (5 MW)
without magnetic field (5 MW)
background (1 MW)

1

0

30

40

50

Scattering angle 2θ (degree)

Fig. 2. Neutron diffraction patterns of iron and background. Filled and open circles denote the diffraction patterns of iron with and without a magnetic field, respectively. Filled squares is the diffraction patterns of background.

31007

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&2

:KDW([LVWVLQDQPVL]HG0ROHFXODU&DVSXOH$VVHPEHOGLQ:DWHU"

Y.-Y. Zhan1, N. Sato, K. Morishima, M. Sugiyama and S.
Hiraoka1,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
'HSDUWPHQWRI%DVLF6FLHQFH7KH8QLYHUVLW\RI7RN\R,1752'8&7,21 Molecular capsules and cages
provide a confined nano-space in which sensing, stabilization, activation, reaction, and catalysis can be realizedbased on the selective encapsulation of target moleculesin their cavity. Previously, we developed cube-shaped
molecular capsules (nanocubes), which are assembled
from six gear-shaped amphiphiles (GSAs) in water.[1]One of the nanocubes, %0, shows high thermal[1-3] andkinetic[4] stabilities, though the GSAs are not connectedby strong chemical bonds but only mesh each other. The%0 nanocube has a 1-nm-sized hydrophobic cavity, inwhich various neutral and anionic species are encapsulated.[1,3,5] The thermodynamic parameters for the encapsulation of anions in the nanocube were previously determined by ITC measurements, and the encapsulation isenthalpically favorable but entropically unfavorable.
However, to correctly interpret the thermodynamic parameters, it should be clarified what exist(s) in the cavityof the nanocube before the encapsulation. Consideringthat the %0 GSA is a dicationic molecule with Cl– as
counter anions, water molecules and/or Cl– anion(s)would be trapped in the nanocube. In this research, SAXS
measurements of the %0 nanocube with and without
NaCl were carried out, which enabled us to discuss what
exist in the cavity of the nanocube.

pure water is 9.6 ± 0.3 Å. As the peak positions of the
SAXS profiles of the two are almost same, the change inthe 5g values with and without NaCl would arise from thedifference in the environment of the cavity of thenanocube not from change in the size of the nanocube.
Indeed, the simulation of the SAXS profiles by changing
the size or the shape of the nanocube caused the shift ofthe prominent peaks, and the SAXS profile of thenanocube in 100 mM aq. NaCl could not be well reproduced by simulation. These results strongly suggest that
Cl– anion(s) should be encapsulated in the nanocube in
100 mM aq. NaCl. In other words, the cavity of thenanocube in pure water should be filled with water molecules. Therefore, the encapsulation occurring in the %0
nanocube can be described as the exchange of watermolecules filled in the cavity with the guest molecule(s),so the release of unstabilized water molecules in the
nanocube contributes to the encapsulation of anions.

(;3(5,0(176 SAXS profiles were measured witha laboratory SAXS instrument (Rigaku NANOPIX) installed at Institute for Integrated Radiation and Nuclear
Science, Kyoto University. X-ray wavelength was 1.54 Å
and the typical sample-to-detector distance was 350 and
95 mm. A sample of the nanocube was prepared by dissolving solid sample of %0 GSA in Milli-Q water. The
concentration of the nanocube was determined by UV
spectroscopy before the SAXS measurements of thenanocube in pure water and in 100 mM NaCl aqueous
solution.
5(68/76 The SAXS profiles and the Guinier plots
for the BM nanocube in pure water and in 100 mM NaClsolution are shown in Figure 1. In our previous study of
the SAXS measurements, two prominent peaks were observed for the nanocubes, which suggests that a discrete
structure is formed in water and that the discussion on the
precise structure of the nanocube is possible based on theposition and the intensity of the peaks. It was found that asimilar SAXS profile was observed irrespective ofwhether NaCl (100 mM) is added or not but that the radius of gyration (5g) of the nanocube determined by theGuinier plot is largely affected by the salt. 5g of thenanocube in 100 mM NaCl is 7.3 ± 0.3 Å, while that inFig. 1. (a) SAXS profiles of a solution of the %0 nanocube inwater with and without NaCl (100 mM). (b) The Guinier plots
for the SAXS data.

5()(5(1&(6[1] Y.-Y. Zhan HWDO, &RPPXQ&KHP,  (2018) 14.
[2] Y.-Y. Zhan HW DO, &KHP (XU -,  (2019)9130–9135.
[3] Y.-Y. Zhan HWDO, 1DWXUH&RPPXQ.,  (2018) 4530.
[4] Y.-Y. Zhan HWDO, 1DWXUH&RPPXQ.,  (2019) 1414.
[5] Y.-Y. Zhan HWDO&RPPXQ&KHP,  (2019) 107.

31009

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&2'DPDJH(YROXWLRQLQ1HXWURQLUUDGLDWHG0HWDOVGXULQJ
1HXWURQ,UUDGLDWLRQDW(OHYDWHG7HPSHUDWXUHVI. Mukouda and Q. Xu1+LURVKLPD,QWHUQDWLRQDO8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  It is accumulated an attention thata damage structure in neutron irradiated metals differs if
the temperature is varied during irradiation [1]. Especially effect of lower temperature irradiation on the development of damage structure in metals which are irradiated subsequently at higher temperature was reported to beremarkable because the point defects nucleate at lower
temperature more frequently during an irradiation. Recently the temperature controlled irradiation devices weredeveloped at KUR [2]. It becomes possible to irradiatecontinuously at two stage of temperature. In the present
work, effects on damage formation in neutron-irradiatedcopper for the temperature variation were examined for
an irradiation at low fluence regime.
(;3(5,0(176 Copper disks of 3mm in diameter
were prepared with 99.999% nominal purity specimen.
Before an irradiation, they were annealed for 5 hours at
1273 K in vacuum of 10-5 Pa. Specimens were irradiatedby fission neutrons in a temperature controlled irradiation
device in KUR-SSS. In the previous temperature varying
irradiation, specimens were irradiated at first at 473K and
573K. After a radiation cooling, they were observed byelectron microscopy. A TEM observation was carried out
using g = (002) reflection with (g, 5g) condition for the
specimens of (110) configuration. Voids were observed ina bright field image by taking a slightly under forcussed
image. A triangular image was taken as stacking fault
tetrahedra (SFT) and diffused dot image was tentatively
taken to be an interstitial cluster.
Present temperature varying irradiation, specimens were
irradiatedat473K-6hrs/573K-40hrs,
473K-23
hrs/573K-23 hrs and 473K-6 hrs/573K-20 hrs at 1MW.
TEM observation are carried out recently.
5(68/76 In 473K-10hrs/573K-10hrs irradiation at
5MW, the number density of voids and SFT was smaller
than those of constant temperature irradiation at 573K.
Especially the decrease of number density of voids was
significant [3]. shows dislocations in the specimen. Dislocations were not decorated by interstitial clusters. The
number density of SFT was smaller than the value incopper which were irradiated at constant temperature of
573 K. Only one void was observed in specimens as inthis picture, which means the formation of voids was
suppressed significantly by the present temperature elevation irradiation.
Neutron-irradiated copper at 573K for 10 hours at 5MW,
the dislocation structure show no decorated interstitialclusters around dislocation. Interstitial clusters, whichwere accumulated along dislocation lines, were unified to
grow to dislocations. This makes development of complicated structure of dislocations as reported by Mukouda
and Shimomura [4].
The suppression of void formation in temperature-varied
irradiation suggests that the nucleation of voids during a
constant temperature irradiation at 573K in copper occurs
during the period of dislocation decoration by interstitialclusters.
In 473K-6hrs/573K-40hrs irradiation at 1MW, the number density of voids and SFT was significant smaller thanthose of constant temperature irradiation at 573K asshown in Fig. 1. Only one void were observed. TEM observation of other irradiation condition specimens areprogress at the present.
5()(5(1&(6[1] N. Yoshida, Q. Xu, H. Watanabe, Y. Miyamoto and T.
Muroga, J. Nucl. Mater., 212-215 (1994) 471.
[2] T. Yoshiie, Annual Reports of KUR (1998).
[3] I. Mukouda and Q. Xu, KURNS progress report 2018,
Co4-7.
[4] I. Mukouda and Y. Shimomura, Material Science &Engineering A309-310 (2001) 190-197.

Fig. 1. Damages observed in neutron-irradiated copperwith temperature varying schedule. The irradiation was
carried out at first at 473K for 6 hours and subsequently
at 573 K for 40 hours at 1MW.

31041

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5DGLDWLRQ5HVLVWLYLW\RI)HUULWH3HUPDQHQW0DJQHWV$JDLQVW1HXWURQVY. Iwashita1, M. Abe1, T. Yako1, T. Kurihara2, M. Fukuda2,
M. Sato2, T. Sugimura2, Y. Iinuma3, Y. Fuwa4,
Y. Kuriyama3 and K. Takamiya3,QVWLWXWHIRU&KHPLFDO5HVHDUFK.\RWR8QLYHUVLW\$FFHOHUDWRU/DERUDWRU\.(.,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
-3$5&&HQWHU-$($,1752'8&7,21  Permanent magnets are used asmaterial of beam optical elements. While rare earth magnets, such as NeFeB and SmCo, are known to have radiation demagnetization [1], there is not enough information
for ferrite magnets, which are economical but have lessremanent field strength. In order to verify the resistivityof ferrite magnets, we carried out a trial experiment on radiation demagnetization of ferrite magnets irradiated byneutrons at Kyoto University Research Reactor (KUR).
(;3(5,0(176 We acquired cylindrical anisotropic
ferrite magnets with 5 mm diameter and 2 mm length thathave easy-axis parallel to the cylinder axis. They are
popular off-the-shelf Y30H (Strontium Ferrite magnets).
Since they seemed to have common non-uniformity on theeasy-axis and they were randomly magnetized, they werere-magnetized to have better magnetic uniformity. We
measured their magnetic field at both end surfaces with aTesla meter (SENIS 3MH3) using a magnet fixture jig prepared for this experiment. The jig has a 0.5 mm thickplastic plate between the Hall probe and the magnet end
surface to avoid a direct contact between them. Since theHall probe measurement is sensitive to the positioning error of magnets, another measurement method was developed. This rotates the small magnet in a coil and the amplitude of the induced voltage is taken. This method isless sensitive to the positioning error.
The irradiation times were 46 hours at 1 MW operation
and 6 hours at 5 MW operation (HYD), and 4 weeks (LongTerm). In these two irradiation conditions, estimated values of thermal neutron fluence on the samples are 5.71018 [n/cm2] and 8.61018 [n/cm2], respectively. A permanent magnet samples packed in aluminum sheets wasplaced into a capsule together and sent to the reactor. After the residual radioactivity of the magnet and capsule decayed sufficiently, we took out the magnet samples fromthe capsule and measured the magnetic field. We compared the magnetic field strength before and after the irradiations.
5(68/76 Fig. 1 shows the ratios of the magnetic fieldstrength before and after the irradiation. The error bars
show the standard deviations of measured data for eachmagnet.
The broken vertical green line in Fig. 1 denotes neutron

dose at which radiation demagnetization becomes significant for NeFeB magnets [1]. Ferrite magnets were foundto be more resistant to the radiation than NeFeB magnets.
According to the data taken so far, the characteristic radiation demagnetization dose is estimated about 1.41020[n/cm2]. Because of the regression function form, thedata points at less radiations have almost no effect on thefitting result. The magnetization will be degraded to half
at dose of about 11020 [n/cm2].
3(563(&7,9(6 The radiation hardness level of ferrite magnets close to those for SmCo magnets is an important information for communities handling radiations.
The ferrite magnets would be widely used in such applications.
More irradiation dose with improved magnetic fieldmeasurement procedure clarified the demagnetization as afunction of the dose level. Measurements on other magnets
such as NdFeB and SmCo magnets with the same procedure is planned for a systematic understanding on the radiation demagnetization on practical magnet materials.

Fig. 1: Ratio of radiation demagnetization of ferrite permanent magnet.
5()(5(1&(6[1] X. -M. Marechal, T. Bizen, Y. Asano, H. Kitamura,
Proceedings of EPAC, Edinburgh, Scotland, 2006.

31042
‑154‑

&2(OXFLGDWLRQRIWKH0HFKDQLVPRIWKH 6FUHZVHQVH,QGXFWLRQRI3RO\PHU%DFNERQH
%DVHGRQWKH6PDOO$QJOH;UD\6FDWWHULQJDQG'\QDPLF/LJKW6FDWWHULQJ0HDVXUHPHQWVY. Nagata1, M. Suginome2, M. Sugiyama3, R. Inoue3, N.
Sato3, and K. Morishima3

QENS measurements by using the results of the DLS
measurements.

,QVWLWXWHIRU&KHPLFDO5HDFWLRQ'HVLJQDQG'LVFRYHU\+RNNDLGR8QLYHUVLW\*UDGXDWH6FKRRORI(QJHQGHULQJ.\RWR8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQDQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Increasing attention has focusedon the structural control of helical polymers owing totheir potential applications for asymmetric catalysts, chiral stationary phase, and chiroptical materials. Recently,
we
found
that
single-handed
helicalpoly(quinoxaline-2,3-diyl)s (PQXs) bearing chiral side
chains exhibit a solvent-dependent helix inversion,1-3
which can serve as effective scaffold for chirality-switchable materials. 4-7 To elucidate the mechanismof the helix inversion of PQXs, we have investigated thedetailed structures of a PQX (100mer) with right- or
left-handed structures in tetrahydrofran-G8 (THF-G8) or amixed solvent of 1,1,2-trichloroethane-G3 (1,1,2-TCE-G3)
and THF-G8 (4/1, v/v) by using small-angle neutron scattering (SANS) experiments, in conjunction with theoretical calculations.8 The obtained structures of the PQX
suggested that the right-handed structure in THF-G8 iswell solvated, while the left-handed structure in
1,1,2-TCE-G3/ THF-G8 (4/1, v/v) is less solvated.
Our recent interest has focused on the impact of the
dynamics of the side chains on the screw-sense induction.
So far, we have carried out quasielastic neutron scattering(QENS) measurements to elucidate the impact of themolecular dynamics on the solvent-dependent helix inversion of the PQX at BL-02 DNA in J-PARC. In thisstudy, we have carried out dynamic light scattering (DLS)
measurements for the detailed analysis of the results of
the QENS measurements.
(;3(5,0(176A
PQX
bearing(5)-2-octyloxymethyl side chains (100mer) was preparedaccording to our previous paper. The light scattering
measurements were carried out with a 22-mW He-Ne
laser, an Avalanche Photo Diode (APD, ALV, Germany)
mounted on static/dynamic compact goniometer,
ALV/LSE-5003 electronics, and ALV-5000 Correlator(ALV-Laser Vertriebsgesellschaft GmbH, Langen, Germany). The measurements were performed at 313 K and
CONTIN analysis was used to obtain the probability of
decay rate at each 4.
5(68/76 The PQX was dissolved in THF-G8 or amixed solvent of 1,1,2-trichloroethane-G3 (1,1,2-TCE-G3)
and THF-G8 (4/1, v/v), respectively, to carry out DLS
measurements (Fig 1). In the both cases, the decay constant ī and the square of the wave vector T2 showed linear relationship, affording the diffusion constants in thesesolvents. We are now working on the analysis of theFig. 1 Correlation between the decay constant ī and thesquare of the wave vector T2. The measurements werecarried out using solutions of the PQX in THF-G8 (blue)
or a mixed solvent of 1,1,2-trichloroethane-G3(1,1,2-TCE-G3) and THF-G8 (4/1, v/v, red).

5()(5(1&(6(1) Yamada, T.; Nagata, Y.; Suginome, M. &KHP
&RPPXQ , , 4914-4916.
(2) Nagata, Y.; Yamada, T.; Adachi, T.; Akai, Y.;
Yamamoto, T.; Suginome, M. - $P &KHP 6RF ,, 10104-10113.
(3) Nagata, Y.; Nishikawa, T.; Suginome, M. - $P
&KHP6RF , , 4070-4073.
(4) Nagata, Y.; Nishikawa, T.; Suginome, M. &KHP
&RPPXQ , , 11193-11195.
(5) Nagata, Y.; Takagi, K.; Suginome, M. - $P &KHP
6RF , , 9858-9861.
(6)Nagata, Y.; Uno, M.; Suginome, M. $QJHZ&KHP,QW
(G , , 7126-7130.
(7) Nishikawa, T.; Nagata, Y.; Suginome, M. $&60DFUR/HWW , , 431-435.
(8) Nagata, Y.; Nishikawa, T.; Suginome, M.; Sato, S.;
Sugiyama, M.; Porcar, L.; Martel, A.; Inoue, R.; Sato, N.
- $P&KHP6RF , , 2722-2726.

31051

‑155‑

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was exposed to γ-ray or X-ray radiations. The γ-ray irradiation experiments were performed with 60Co γ-ray at
the Co-60 Gamma-ray Irradiation Facility at Institute forIntegrated Radiation and Nuclear Science, Kyoto University. The irradiation dose was represented as absorbed
dose for water. The X-ray irradiation was performed using an X-ray source with a Rh target.

Y. Takada, R. Hashikawa, Y. Nishi, A. Kinomura1, T.
Saito1, A. Okada2, T. Wakasugi2, K. Kadono2
Graduate School of Science and Technology,
Kyoto Institute of Technology
1Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Faculty of Materials Science and Engineering,
Kyoto Institute of Technology.

INTRODUCTION: Radiophotoluminescence (RPL) isa luminescence phenomenon in a material induced byexposure to high-energy radiation. Silver-activatedphosphate glasses are well known as a material exhibiting
the RPL phenomenon, and these glasses are applied for a
personal dosimeter [1]. However, only a few materials
have been found to have a prominent RPL other than thesilver-activated phosphate glasses. Thus, extensive exploration is performed to obtain materials having highperformance RPL behavior. We have reported that inaluminoborosilicate glasses doped with an extremely low
content of copper, intense photoluminescence is inducedby the exposure of the glasses to X-ray and γ-ray irradiation [2]. The mechanism of the RPL phenomenon for the
Cu-doped glass is considered to be as follows [2]:Copper in the glass mainly exists as divalent Cu2+ ormonovalent Cu+ ions. The former, Cu2+ ion, has no luminescence while the latter, Cu+ ion, has a bright one
around 500 nm by the excitation at 240 nm. When theglass doped with copper is exposed to high-energy radiation, electron and hole pairs are generated in the glass as
expressed by (1) and a part of them are captured by Cu2+
and Cu+ ions, respectively as equations, (2) and (3).
(1)
Glass ĺ h+ + e−(2)
Cu2+ + e− ĺ Cu+(3)
Cu+ + h+ ĺ Cu2+
When the electron capture process (2) is more predominant than the hole capture process (3), the concentrationof the luminescence species, Cu+, increases and as a result, the luminescence will increase.
We have investigated the RPL behaviors ofcopper in other glass systems. Here, we report the photoluminescence behaviors of Cu-doped silica glass that was
prepared through the immersion of a porous silica glassin a Cu(NO3)2 aqueous solution using the glass as a starting material [3].
EXPERIMENTS: The porous silica glass used as astarting material was prepared from a phase-separated
borosilicate glass with a composition, 9.0Na2O 㺃
26.6B2O3 㺃64.4SiO2. The porous silica glass was immersed in 0.0005 to 0.005 M Cu(NO3)2 aqueous solution
to dope copper into the porous silica glass. The Cu-doped
porous silica glass was sintered at 900°C for 2 hours, andcut and optically polished to 1 mm thickness. The
Cu-doped silica glass (abbreviated as Cu-SG, hereafter)

RESULTS: Figure 1 shows the photoluminescence
spectra of the 0.0005 M-Cu-SG silica glass (prepared by
the immersion in 0.0005 M Cu(NO3)2 solution) measured
before and after the γ-ray irradiation with the intensity of
approximately 800 Gy and the appearance of the glass
under the UV-radiation. The spectra and the appearanceof the 0.005 mol% Cu-doped aluminoborosilicate glass(abbreviated as Cu-ABS25) was also shown for comparison. Both spectra after the irradiation are normalizedwith the intensity of the spectra before the irradiation,
respectively. The photoluminescence intensity for the
Cu-SG increased approximately two times by the irradiation (see the solid line arrow) while that for the
Cu-ABS25 increased four times (dotted line arrow). The
spectrum of the Cu-SG shifted to the longer wavelength
direction after the irradiation and the color of the luminescence varied from blue to yellow. This is due to thedifference in the coordination environment of the Cu+
generated by the electron capture from that of the Cu+
existing before the irradiation as the glass prepared.

Fig. 1. Emission spectra of Cu-doped glasses(Cu-SG and Cu-ABS). The spectra were normalizedwith the peak intensities of the spectra before irradiation.
The intensity of photoluminescence after
the irradiation was proportionally increased with the absorbed dose. The ratio of the intensities after and before
the irradiation decreased with the concentration of copper
incorporated into the glass.
REFERENCES:>@ R. Yokota, et al., J. Phys. Soc. Jpn., 23 (1966)
1038-1048.
>@ H. Hashikawa, et al., J. Am. Cer. Soc., 102(4) (2019)1642-1651.
>@ D. Chen, et al., Appl. Phys. Lett., 86 (2005) 231908.

31066

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M . Kobayashi, T . Miyachi , S . Takechi1, Y. Morita1,
A. Umehara2, Reo Kunimatsu2 and Ryo Sasaki2
3ODQHWDU\ ([SORUDWLRQ 5HVHDUFK &HQWHU &KLED ,QVWLWXWH
RI7HFKQRORJ\*UDGXDWH6FKRRORI(QJLQHHULQJ2VDND&LW\8QLYHUVLW\'HSDUWPHQWRI(QJLQHHULQJ2VDND&LW\8QLYHUVLW\,1752'8&7,21  In the previous years, we havefound that when irradiating high intensity heavy ions to apiezoelectric element (400 MeV/n Xe beam at HIMAC of
the National Institute of Radiological Sciences [1][2]), its
resonance frequency and anti-resonance frequency are
shifted and also the impedance at the resonance frequency and anti-resonance frequency are changed by beamirradiation and then the electromechanical coupling coefficients of those piezoelectric elements were decreased.
There are two types of radiation damage to generalmaterials, due to ionizing and non-ionizing dose effects(or displacement damage). Since the piezoelectric element is a crystalline material, it is considered that the
crystal is damaged by the beam irradiation and thus thecharacteristic parameter such as the resonance frequency
has changed. However, detailed mechanism such as its
mechanism is not known.
Therefore, in this study, we investigated the responseof the piezoelectricity against energetic electron beamirradiation which has dominantly ionizing effect (lessnon-ionizing effect) to compare with the previous results.
(;3(5,0(176 $1' 5(687/6 In this year, we
had two experiment campaigns for electron beam irradiation to piezoelectric PZT elements in KURRI-LINAC.
 7KHILUVWH[SHULPHQWRQ0D\WRLQ In theexperiments up to the previous year, we found that thedecrease in piezoelectricity due to electron irradiation
was smaller than that due to xenon irradiation. Therefore,
we devised an experiment setup to improve the quality ofthe experiment in order to have more quantitative discussion. The setup of irradiation target holder and positioning mechanism has been improved for more precise positioning against the electron beam because results weresometimes varied even if the beam condition was thesame. As the results, the change of the electromechanicalcoupling coefficients of irradiated PZT targets against thecurrent of electron beam became less variable.
We have monitored the temperature on the surface ofthe target piezoelectric elements which were cooled byforced air cooling during electron irradiation to the elements because the piezoelectricity can be lost or reducedby heat when the temperature becomes close to its Curie
point. We estimated the internal temperature of the target
piezoelectric elements with a thermal analysis taking into
account of the forced air cooling and noticed that the internal temperature can be higher than the surface one. We
performed how the piezoelectricity is reduced by temperature by using a thermostatic chamber and obtained afunction of “piezoelectricity loss” of the piezoelectricelement as temperature.

(2) 7KHVHFRQGH[SHULPHQWRQ-DQXDU\WRLQ:We performed the second electron irradiation experiment
so that the internal temperature may not become over the
point at which the piezoelectricity begins to be reduced,
by monitoring the surface temperature of the target ones.
As the results, we could measure the net reduction inpiezoelectricity due to electron beam irradiation. An experiment was conducted in which one specimen was irradiated with an electron beam for 15 hours or more, which
we had never done previously because it was difficult toensure the reproducibility of the experiment before thisexperiment.
We confirmed that the electromechanical coupling
coefficient changes in the experiment of electron beam
intensity, which is considered to be the effect of radiation
only. For more better measurement, we used the othercable to connect the target piezoelectric with the measurement devices of impedance analyzer to exclude theeffect of the capacitance of the cable and then we foundthat the measurement results vary depending on the cableattached to measure the piezoelectricity of the piezoelectric element. We will improve the situation in the future.
In this experiment campaign, we measured gamma
rays emitted from radio-activated target piezoelectricmaterial. That radioactivity may be produced by neutrons
created by energetic electron. In order to determine thenet effect of electron irradiation, we will evaluate theeffect of radiation damage by neutron by analyzing the
gamma ray spectra that we obtained in the experiments.
6800$5< $1' )8785( 35263(&76 In the experiments up to the previous year, we had difficulty toensure reproducibility such as the alignment of the target
with respect to the electron beam, but we were able toestablish an experimental setup for high-precision measurement. As a result, we were able to specify a certain
temperature point distinguish only the effects of radiation
irradiation to piezoelectricity decrease. There is a problem with the cable for measurement, but we will solve theproblem for experiments in the next experiment campaign for more further accurate measurements.
5()(5(1&(6>@ M. Kobayashi et al., Japanese Journal of Applied
Physics 53, 066602 (2014).
>@ M. Kobayashi et al., Japanese Journal of Applied
Physics 52, 126604 (2013).

31067

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)RUPDWLRQRIUDGLDWLRQGHIHFWVRQWXQJVWHQDQGWKHLULQIOXHQFHRQHIIHFWRIK\GURJHQLVRWRSHUHWHQWLRQ

5HVHDUFK,QVWLWXWHIRU$SSOLHG0HFKDQLFV.KXVKX8QL
YHUVLW\+\GURJHQ,VRWRSH5HVHDUFK&HQWHU8QLYHUVLW\RI 
7R\DPD,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  It is of a great importance to clarify phenomena of implantation, retention, diffusion andpermeation of tritium (T) on surface of the armor materials of the first wall/blanket and the divertor on fusion
device from a viewpoint of precise control of fuel particles, reduction of tritium inventory and safe waste management of materials contaminated with tritium. Refractory metals such as tungsten (W) is potential candidate
for the armor of the first wall and the divertor plate of thefusion reactor because of its low erosion yield and goodthermal properties. The armor material will be subjected
to heavy thermal loads in the steady state or transientmode combined with high energy neutron irradiation thatwill cause serious material degradation. In addition, highenergy runaway electrons would bombard the armor materials along the equatorial plane in fusion device. It isconsidered that these cause radiation damage and enhance tritium retention. In the present works, T exposure
experiments have been carried out on W samples whichwere irradiated by high energy electrons to investigate
effects of high energy electrons irradiation on microstructure and tritium retention of W. In this fiscal year,
pure W and recrystallized W were irradiated by highenergy electron beam. Before and after that, positronannihilation experiment was carried out to identify theradiation defect. In addition, EBSD 㸦 Electron Back
Scatter Diffraction Patterns㸧analyses has been carriedout on the specimens before and after the electrons irradiation. Tritium exposure experiments have been carriedout using a tritium (T) exposure device.
(;3(5,0(176 W samples used were ITER specification W (ALMT-grade) (SR-W) and its recrystallized
W (RC-W). The SR-W was fabricated via a powder metallurgical route including cold isostatic pressing, sintering, hot rolling, and heat treating to relieve the residual
stresses. Some of the machined SR specimens were subjected to a full recrystallization treatment at 2000 ºC for
1 hr in vacuum. Sizes of the specimens were 10 mm x 10mm x 1mm (10 mm x 10 mm : ND-TD). The surfaceof the both samples were polished to be mirrored㸬 Highenergy electrons irradiation has been carried out using
LINAC in Institute for Integrated Radiation and Nuclear
Science, Kyoto University. An peak energy of electron
irradiated was 8 MeV and DPA was 5.8 x 10-3. Temperature during the irradiation was measured by thermocou-

ples which was contacted with a backside of the W samples. Before and after that, positron annihilation experiment was carried out to identify the radiation defect. In
addi-tion, EBSD㸦Electron Back Scatter Diffraction Patterns㸧analyses has been carried out on the specimens
before and after the electrons irradiation. T exposure experiments have been carried out using a T exposure device in University of Toyama. Pressure of the T gas was
1.3 kPa and T exposure was kept for 4 h. T concentrationin the gas was about 5 %. Temperatures of pre-heating
and T exposures were 100 oC and 100 oC. After the exposure to T gas, T amount retained in surface layers of
the sample was evaluated by ș-ray-induced X-ray spectrometry (BIXS) and imaging plate (IP) measurements.
5(68/76 As shown in Fig. 1, mean lifetime from
RC-W is smaller than that from SR-W. After the e irradiation, mean lifetime of both increases. τ1 and τ2 from the
SR-W is bigger than that from RC-W. In addition, I2 from
RC-W is bigger than that from SR-W. Because τ2 of
RC-W after the e irradiation is 266.1 ps, defects are considered to aggregate by temperature increase due to theirradiation.

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K. Tokunaga, M. Matsuyama1, M. Hasegawa,K. Nakamura and Q. Xu2

㻔㼍㻕
㻟㻜㻜
㻞㻜㻜
㻝㻜㻜
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㼕㼞㼞㼍㼐㼕㼍㼠㼕㼛㼚

㻵㻞

㻠㻜
㻞㻜

Fig. 1.

‑160‑

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㻜

31086

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㼕㼞㼞㼍㼐㼕㼍㼠㼕㼛㼚

Positron life time(a) and intensity of I2 (b).

&2

Tritium release behavior from neutron-irradiated FLiNaBe

K. Katayama, K. Kubo, K. Tsukahara, A. Ipponsugi, M.
Oya, T. Takeishi1, S. Fukada, and Y. Iinuma2

each bubbler was sampled periodically to observe thechanges with time in release rates of TF and HT. After theexperiment was finished, the temperature was increased
to room temperature and cumulative HTO in the cold trap
was purged by Ar and it was collected in a new water
bubbler.

Department of Advanced Energy Engineering Science,
Kyushu University
1
Faculty of Engineering, Kyushu University
2
Institute for Integrated Radiation and Nuclear
Science, Kyoto University

Heater

H2 → H2O
for water vapor purge

CuO

Cold-trap(Ethanol with dry ice)

T2O
or
HTO

MFC
TC

T2 → T2O
HT → HTO
HeaterCuO

FLiNaBe

H2

+

Ar

Ar
HeaterMo
Crucible

TF

T2 or HT

Fig.1 The schematic of experimental apparatus.
RESULTS: Fig.1 shows cumulative HT and TF released from neutron irradiated FLiNaBe in the initialheating to 600 ℃. As shown in Fig.1, most tritium wasreleased as HT. After cooling the temperature below themelting point, the heating at 700 ° C was performed again.
As a result, the release rate of TF gradually increased,
and the rates of TF and HT reached the same degree. Initially tritium would be presence as TF in FLiNaBe but
after melting TF was considered to react with Mo on the
crucible and Fe on the reaction tube and converted to T2.
It can be said that as the fluoridation on the metal surface
progressed, the reduction reaction of TF decreased, andthe release rate of TF increased. This result suggests thepossibility of redox control of TF by Mo. The releaseratio of each chemical form was approximately TF: HT:
HTO = 30:64:6. The majority of tritium was released as
HT (or T2). This result indicates that corrosion of metals
by TF occurred in tritium release process. In the next
experiment, the effect of H2 purge on the suppression of
corrosion will be investigated.

‑161‑

600

Temperature

80

500

HT or T2

400

60

300

40

200
20
0

TF

0

20

40

60
80
Time [min]

100

o

31090

100

Temperature [ C]

EXPERIMENTS: In the powders of LiF, NaF and
BeF2 were mixed in a Ni crucible under Ar atmosphere.
The Ni crucible was put in the stainless-steel heating pot
and repeatedly heated to 500 ℃ with Ar purging to remove impurity water vapor. The heating was repeated tohomogenize the FLiNaBe. The prepared sample of
FLiNaBe was packed into polyethylene bag with Ar gas
and it was installed into a capsule. The thermal neutrons
irradiation was performed by at pneumatic tube 2 (Pn-2)
in Kyoto University Research Reactor with the fluence ofat Pneumatic Tube 2 (Pn-2) of the 1.7×1015 cm-2.
Tritium release experiment was carried out in Kyushu
University. The schematic illustration of experimental
apparatus is shown in Fig.1 The irradiated sample wasput in a Mo crucible and it was installed in the stainless-steel reaction tube. The sample was heated to 600 ℃
with Ar purge. The chemical form of tritium released
from the sample was expected to be TF and HT (T2) andHTO (T2O). In this experiment, since HT and T2, HTO
and T2O cannot be distinguished, here these are represented as HT and HTO, respectively. HTO was collected
in a cold trap, which was a spiral cupper tube immersed
in ethanol with dry ice. TF was collected in a first water
bubbler, and HT were collected in a second water bubbler
after conversion to HTO by a CuO bed. The water of

MS3A

Cumulative released tritium [kBq/g]

INTRODUCTION: FLiNaBe, which is a mixed molten salt of LiF+NaF+BeF2, is a promising liquid blanket
material for a fusion reactor [1]. Tritium is produced in
FLiNaBe by the nuclear reaction between neutrons and
Li in the blanket. In the self-cooling system where thetritium breeding material itself transport heat to the heatexchanger, FLiNaBe plays two important roles of tritiumtransport and heat transport. Since FLiNaBe have a low
solubility for hydrogen isotopes, the generated tritium
tends to release from FLiNaBe. This property means that
tritium can be easily recovered from FLiNaBe but also apart of tritium is lost to the outside of cooling tubes by
the permeation on the way to the tritium recovery system.
In order to control tritium safely and to design tritium
recovery system, it is necessary to understand the fundamental behavior of tritium generated inside FLiNaBe
by nuclear rection. In this study, the solid state sample of
FLiNaBe was irradiated by thermal neutrons at Kyoto
University Research Reactor, and tritium release behavior from the free surface of FLiNaBe by heating was observed in Kyushu University.

100
0
120

Fig.2 HT, T2 and TF release from irradiated FLiNaBe.

&2 Positron Age-Momentum Correlation Mesurements of Ȗ-rays Irradited Polystyrene
H. Tsuchida1,2, S. Konishi2, Q. Xu3

increases linearly with dose, and there is a clear correlation between the S parameter and Ȗ-rays radiation dose.

1

Quantum Science and Engineering Center, Kyoto University
2
Department of Nuclear Engineering, Kyoto University
3
Institute of Integrated Radiation and Nuclear Science,
Kyoto University

0.47

EXPERIMENTS: The experiments were performed at
the Co-60 Ȗ-rays irradiation facility of KURNS. Polystyrene was used as a target specimen. The specimens with athickness of 2-mm were irradiated with Co-60 Ȗ-rays
with energies of 1.17 and 1.33 MeV at various doses of30, 200, 300 and 400 kGy. The irradiation experiments
were performed at room temperature. The dose rate was
10 kGy/h. In the specimens after irradiation, we analyzed
the resultant damage using ȕ+íȖ based AMOC measurement system with Ge-68 positron source.
RESULTS: Based on the observed AMOC spectrum,
we obtained variation of S parameter as a function of
positron age (t), where S corresponds to the positron annihilation Doppler Broadening, which is defined as theratio of the counts in the central position of the annihilation photopeak to the total counts in the peak. Figure 1
shows typical results. In this figure, S parameter at time
region t = 0í3 ns corresponds to annihilation of free positrons or para-positronium (p-Ps). S at t > 3 ns corresponds to the pick-off annihilation of o-Ps formed in thefree volume of polystyrene. The behavior strongly depends on the radiation dose, and the S parameter significantly decreases with increasing dose.
The S parameter of o-Ps is attributed to interactions ofo-Ps with low-momentum electrons near free volume. We
defined an average value of S parameter at time region 3
ns < t < 7 ns as the S parameter for o-Ps pick-off annihilation. Figure 2 shows its dose dependence. One can seethat the S parameter decreases with increasing Ȗ-rays
radiation dose. In this case, the measured lifetime of o-Ps
annihilation (Ĳ3 = 2.03 ns) remains unchanged after irradiation. We found that radiation damage near free volume

31093

‑162‑

0.45
0.44
0.43
0.42
0

1

2

3

4

5

6

7

Time [ns]Fig. 1. Time dependent S-parameter of the o-Ps
pick-off annihilation for before irradiation (Ŷ) andafter Co-60 Ȗ-rays irradiation at different dose: 30
kGy (Ɣ), 200 kGy (Ɣ), 300 kGy (Ɣ), and 400 kGy
(Ɣ).

0.46

o-Ps S parameter

INTRODUCTION: Studies on the irradiation-induced
damage in polymers are of technical importance for developing radiation-resistance materials. In this work, weinvestigate microstructure changes of free volume inpolystyrene induced by Ȗ-rays irradiation at high dose.
The free volume affects materials properties. The resultant damage was analyzed by the age-momentum correlation (AMOC) positron annihilation technique. The AMOC is a correlated measurement of the positron lifetime(positron age) and the momentum of the annihilating positron-electron pair. We study the radiation-induced damenear free volume of polystyrene via the annihilation processes of ortho-positronium (o-Ps).

S prameter

0.46

0.45

0.44

0.43

0.42

0

100

200

300

J irradiation dose [kGy]400

Fig. 2 Variation of S parameter for the o-Ps pick-off
annihilation as a function of dose. The symbols denote data observed for before (Ƒ) and irradiatedspecimens (Ŷ).

&2

)RUPDWLRQRIQDQRVWUXFWXUHVRQ*HVXUIDFHVE\LRQLUUDGLDWLRQDQG
VWXG\RQLWVIRUPDWLRQPHFKDQLVPVJ. Yanagisawa, R. Tsukamoto1, K. Ishihara, Q. Xu2, A.
Yabuuchi2, K. Takamiya2 and A. Kinomura2

1014 or 1015 cm-2. S parameters were measured using the
KUR slow positron beam system. 

6FKRRORI(QJLQHHULQJ7KH8QLYHUVLW\RI6KLJD3UHIHF
WXUH

5(68/76 DQG ',6&866,21 Figure 1 shows thethree-dimensional atomic force microscope (AFM) images of the Ga+-irradiated surfaces. Figure 2 shows the S
parameters as a function of positron energy for the corresponding samples as shown in Fig. 1. It is found that the
behavior of the S parameter for the 0.5 keV, 1 x 1014 cm-2
Ar+ irradiated surface was almost the same as that for theun-irradiated surface, although the values were unnaturally different each other. This can be supported from thesimilar AFM images, as shown in Figs. 1(a) and 1(d),although the density of the bumps was different. For thelarger Ar+ fluence and irradiation energy, however, thesurface morphology was drastically changed, as shown in
Figs. 1(b) and 1(c). This might be relevant to the drastic
increase in the S parameters for them.

1*UDGXDWH 6FKRRORI(QJLQHHULQJ7KH8QLYHUVLW\RI6KL
JD3UHIHFWXUH2,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  We have reported that the formation of swelled nano-porous structures can be formedon Ge surfaces by Ga, Au or Si ion irradiations at theenergy of 100-200 keV, but no such structures were observed by 15-30 keV ion irradiations [1]. We have also
observed the formation of nano structures on the 25-60
keV Ar+-irradiated areas of the Ge (110) surfaces, and themeasurements of S parameters from the Doppler broadening of annihilation gamma-rays as a function of incident positron energy by the KUR slow positron beansystem were performed [2]. The increases of the S parameters were observed for the ion-irradiated surfaces by
the 25-50 keV Ar+ with the ion fluences of 1-5 x 1016
cm-2, showing the formation of atomic vacancies and/or
voids on the ion-irradiated surfaces. On the other hand,
we have found that nano-scale bumps on both Si and
SiO2 surfaces were formed by Ga+ irradiation at an energy of 0.5 or 4 keV. In the present study, such Ga+ irradiation was performed on Ge (110) surfaces and the S parameter was measured.
(;3(5,0(176 Ga+ ion irradiation on the Ge (110)chip surfaces (each size of 1.5 x 1.5 cm2) was performed
using a needle type liquid-metal ion source at the acceleration voltage of 0.5 or 4 kV with the ion fluence of 1 x(a)‫ ڦ‬0.5 keV, 1x1015 cm-2, ‫ ی‬4 keV, 1x1015 cm-2
‫ ڸ‬un-irradiated,‫ ە‬0.5 keV, 1x1014 cm-2(b)Fig. 2. S parameters for low-energy Ga+-irradiated andun-irradiated Ge(110) surfaces as a function of positronenergy.

(c)(d)

Fig. 1. AFM images of Ga+-irradiated (using ion energy and fluence of (a) 0.5 keV and 1x1014 cm-2, (b)0.5 keV and 1x1015 cm-2, (c) 4 keV, 1x1015 cm-2, respectively,) and (d) un-irradiated Ge(110) surfaces. &21&/86,21 Effect of the low-energy Ga ion irradiation on Ge (110) surfaces was studied using S parameters of the slow positron beam measurements. It is foundthat Ga+ irradiation at lower energy (such as 0.5 keV) andlower fluence (1 x 1014 cm-2) makes almost no effect on
the formation of atomic vacancies and/or voids on the Ge
surfaces.
5()(5(1&(6[1] J. Yanagisawa, K. Takarabe, K. Ogushi, K. Gamo andY. Akasaka, J. Phys.: Condens. Matter  (2007)
445002 (10pp).
[2] J. Yanagisawa, Q. Xu, A. Yabuuchi, K. Takamiya, andA. Kinomura, KURNS Progress Report 2018 (Kyoto
University), CO4-9 (30037).

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3RVLWURQ$QQLKLODWLRQ

J. Takahashi2, R. Nakajima3, K. Kitahara1, A. Yabuuchi3,
N. Oshima4, I. Kanazawa2, A. Kinomura3, K. Kimura1

imant crystal have metallic properties. It is of significance to investigate AlPdRu quasicrystal and, AlPdRu
approximant crystals, from the standpoint of structural
vacancy density. In this study, we have measured the
Doppler broadening of quasicrystal AlPdRu, 2/1 approximant crystal AlPdRu, and 1/0 approximant crystal
AlPdRu by the slow positron beam, and also measured
coincidence Doppler broadening(CDB) of 2/1 approximant crystal AlPdRu and 1/0 approximant crystal AlPdRu.

'HSDUWPHQWRI$GYDQFHG0DWHULDOV6FLHQFH7KH8QL
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7HFKQRORJ\ $,67
,1752'8&7,21The thermodynamically stable Al-based icosahedral
quasicrystals, which contain transition metals, have theanomalous electrical-conductivities, such as semiconductor-like properties [1]. However, there is no evidence
for a gap as in semiconductors, and the structure is highlyorderd, although it is no periodic. Mayon et al.[2] proposed a possible explanation for the unusual transport
properties of Al-based quasicrystals in terms of hopping
processed between wave functions mainly localized inside icosahedral clusters. Kimura et al.[3] have discussed
the importance of vacant centers of the icosahedral clusters in the anomalous transport properties and stabilities
of Al-based quasicrystals. They have shown that
12-atoms Al icosahedra with a vacant center have a covalent bonding nature, while 13-atoms with a center atom
have a metallic bonding nature. Kirihara et al.[4] performed an electron density distribution analysis for 1/1
AlReSi approximant crystal and 1/0 AlRe approximant
crystal by the MEM/Rietvelt method, which induced metallic-covalent bonding conversion in Al-based quasicrystals and approximant crystals. Positron annihilation
method is powerful one for detecting structural vacanciesof icosahedral quasicrystals[5]. Recently Kimura andcoworkers [6] have done positron annihilation measurements of the positron lifetime, coincidence Doppler
broadening(CDB), and depth profiling by slow positron
beams for 1/1 AlReSi approximant crystals. They showedthat 1/1 AlReSi approximant crystal has structural vacancies in the order of 10-3, which are identified to be centersites of the first shell of icosahedral clusters, and thenfound that the structural vacancy density of metallic 1/1
AlReSi with less Re is lower than that of non-metallic
AlReSi with more Re. These results accelate further investigation of the relationship between structure, bonding
nature, and electrical properties for 1/1 AlReSi approximant crystals with different Re concentrations, leading tobetter understanding of physics behind quasicrystals andapproximant crystals in terms of the proposed metallic-covalent binding conversion which occurs according
to the occupation and vacany of the center sites of the Al
icosahedral clusters. Tamura et al.[7] have measured theelectrical-conductivities of AlPdRu quasicrystals, 2/1
AlPdRu approximant crystal, and 1/0 AlPdRu approximant crystal. They found very interesting resuls. That is,quasicrystal AlPdRu and 2/1 AlPdRu approximant crystal
have non-metallic properties, while 1/0 AlPdRu approx-(;3(5,0(176DQG5(68/76
By using the slow positron beam, we have estimatedthe change in S-parameter with positron-incident energies
in 2/1 approximant crystal AlPdRu, and 1/0 approximant
crystal AlPdRu. In the case of 1/0 approximant crystal,
S-parameter increases from ~0 to ~ 1 keV. While, in thecase of 2/1 approximant crystal AlPdRu, S-parameterincreses remarkably from ~0 to ~0.5 keV. This means thatthe density of structural vacancies in 2/1 approximant
crystal AlPdRu might be higher than that of 1/0 approximant crystal AlPdRu. These results are consistent withthose of positron lifetimes of approximant crystals 2/1
AlPdRu and approximant crystals 1/0 AlPdRu by slow
positron beams (unpublished data). Furthermore, the present results seem to be reasonable from the standpoint of
the metallic-covalent bonding conversion which occurs
according to the occupation and vacancy of the centersites of the Al icosahedral clusters. Unfortunately, we
could not prepare the sample of AlPdRu quasicrystals. In
order to investigate the relationship between structure,bonding nature, and electrical properties, in Al-based
quasicrystals, positron annihilation measurements of
AlPdRu quasicrystals have been required.
We have done the coincidence Doppler broadening
spectra of 2/1 approximant crystal AlPdRu and 1/0 approximant crystal AlPdRu. To identify the positron trapping sites in 2/1 approximant crystal AlPdRu and 1/0
approximant crystal AlPdRu, the core electron momentum distribution of samples were measured by the coincidence Doppler broadening spectra. Experimental results
suggest strongly that the trapping sites of 2/1 approximant crystal AlPdRu and 1/0 approximant crystal AlPdRu
seem to be Similar.

5()(5(1&(6>@ K. Kimura and S. Takeuchi in Quasicrystals: The
State of the Art, 2nd ed., D.P. Divincenzo and P.J. Steinhart eds., World Scientific, Singapore (1999) pp.325-309.
>@ D. Mayou HWDO Phys. Rev. Lett.  (1993) 3915.
>@ K. Kimura HWDO J. Solid State Chem. (1997) 302.
>@ K. Kirihara HWDO Phys. Rev. Lett. (2000) 3468.
>@ I. Kanazawa HWDO Phys. Rev. Lett. (1997) 2269.
>@ K. Yamada HWDO Philog. Mag. (2018) 107.
>@ R. Tamura HWDOJ. Phys:Condens. Matter  (1999)
10343.

31100

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&2

Absorption Coefficient of Amino Acid in the Sub-THz region using CTR

T. Takahashi,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: Coherent radiation emitted from ashort bunch of relativistic electrons is useful as a bright
light source in the THz-wave and millimeter wave
regions for the spectroscopic purpose. Coherent transition
radiation (CTR), which is emitted from a boundary
between two media, is one of such a coherent light source.
CTR is usually utilized as a non-polarized light source,
because the electric vector of transition radiation (TR)emitted from a metallic screen is axially symmetric withrespect to the trajectory of an electron beam. In thiswavelength range, it is difficult to generate the circularly
polarized light because of the property of the opticaldevice. In my previous reports [1] the circularly polarized
CTR using a pair of wire-grid radiators with the different
polarization has been developed with a new idea. The
significant point of my new technique is the use of
linearly polarized CTR with the wire-grid radiator. With
this technique the polarization degree is able to becontrolled precisely. Circularly polarized light has been
useful in the circular dichroism spectroscopy. Before
using the light, spectra of some kinds of amino acid havebeen measured using linearly polarized CTR [2]. In thisreport absorption coefficients of them are compared.
EXPERIMENTAL PROCEDURES: The experiment
was performed at the coherent radiation beamline [3] atthe L-band linac of the Research Reactor Institute, Kyoto
University. The energy, the width of the macro pulse, andthe repetition rate of the electron beam were 42 MeV, 47
ns, and 60 Hz, respectively. The average current of theelectron beam was 2.3 PA.

7KH VSHFWUXP RI &75 ZDV PHDVXUHG E\ D
0DUWLQ3XSOHWW W\SH LQWHU IHURPHWHU DQG aliquid-helium-cooled Si bolometer 7KH VFKHPDWLF
GLDJUDP RI WKH H[SHULPHQW ZDV VKRZQ LQ )LJ
Figure 2 is the photograph of the spectrometer and thedetector.
RESULTS: The thickness of these samples was 2 mm.
Calculated absorption coefficient of Ș -Alanine,
Phenylalanine, and Tryptophan, are shown in Figs. 3.
Difference between L and D forms has been observed. Inorder to investigate this discrepancy, it is necessary tomeasure using the circularly polarized light.
REFERENCES:[1] T. Takahashi, et al., .855,35&2.
[2] T. Takahashi, et al., .855,35&2.
[3] T. Takahashi et al., Rev. Sci. Instrum. 69 (1998)
3770.

Fig.2 The photograph around the spectrometer.

Fig.1 The schematic diagram of the experiment.

Fig.3 Absorption Coefficient of some kinds ofamino acid.



‑165‑

&2 9DFDQF\PLJUDWLRQEHKDYLRULQ&R&U)H0Q1LKLJKHQWURS\DOOR\VDQGWKHLUVXEV\VWHPV. Sugita, M. Mizuno, A. Yabuuchi1, A. Kinomura1 and+ Araki*UDGXDWH6FKRRORI(QJLQHHULQJ2VDND8QLYHUVLW\1,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\a Na-22 positron source of 0.5 MBq activity in order toacquire 3 million counts in the positron lifetime spectrum.
The measured spectra were analyzed using the programs
RESOLUTION and POSITRONFIT Extended.

140
CoCrFeMnNi
CoCrFe0.25MnNi
CoCrFeNi
CrFeNi

135
130

125
120
115

110
105
100
0

Non-irrad.
As irrad.

(;3(5,0(176  Vacuum induction melted ingots of
CoCrFeMnNi, CoCrFe0.25MnNi, CoCrFeNi and CrFeNi
alloys were purchased from Koujundo chemical laboratory (Japan). The ingots were homogenized at 1373K for
24 h in silica tubes under Ar atmosphere, and were thenmachined into 10 × 10 × 0.5 mm plate pieces by electric
discharge machining. The alloy ingots were cut into
square plate specimens with dimensions of 10 × 10 × 0.5
mm3. The specimens were subjected to strain relief annealing at 1373K for 10 h and then rapidly cooled toprevent secondary phase precipitation and to stabilize
single-phase FCC structures. The specimens in waterflow were exposed to 8 MeV electron beam irradiationfor 3 h in KURNS-LINAC. The irradiation damage was
evaluated at (1.3 - 1.8) 10-4 dpa. In order to investigate
the thermal stability of vacancies, the electron irradiatedspecimens were subjected to the subsequent isochronalannealing at 373-673 K for 1 h.
Positron lifetime measurements were carried out by using
a digital oscilloscope system with photomultiplier tubes
mounted with BaF2 scintillators, having a time resolution(FWHM) of 180 ps. The positron lifetime measurements
require data acquisition for approximately 15 hours with

5(68/76 The mean positron lifetime after isochronalannealing of the electron irradiated samples is shown in
Fig.1. The positron lifetime spectra of as-irradiated samples show a clear separation into two exponential components of positrons with a long lifetime of 185-195 ps.
This indicates that a part of positrons is trapped by monovacancies or relatively small vacancy clusters introduced by during the electron irradiation. After the subsequent isochronal annealing, the mean positron lifetime isfound to decrease sharply around 473K. This can be attributed to the decrease in vacancy concentrations triggered by the free vacancy-migration. It demonstrates thevacancy migration enthalpy in the CoCrFeMnNi highentropy alloy is very similar to that in the CrFeNi alloy.
These results indicate that the “'sluggish diffusion”
hypothesis is not supported in CoCrFeMnNi high entropy
alloys and their subsystems at least in view of vacancy
migration behavior.

Mean positron lifetime (ps),1752'8&7,21  Alloy design has traditionallybeen done by selecting the base material and adding theappropriate elements to achieve the desired properties. In
the last decade, a new type of multicomponent alloy
called "high entropy alloys" containing equiatomic /near-equiatomic ratios of constituent elements was proposed by Yeh et al [1-3]. These alloys often exhibit
simple solid solution structures at high temperatures dueto the high constituent entropy of random solid solution
mixtures. High entropy alloys have been reported to havepromising properties for practical use, such as highstrength, high fracture toughness, excellent oxidation
resistance and corrosion resistance combined with ductility. A major factor in these properties is thought to be thekinetics of "sluggish diffusion". Therefore, the diffusion
kinetics of high entropy alloys has been actively studied
by diffusion logarithms and tracer diffusion methods, as
the atomic diffusion in a multiprincipal element matrix
has also been of interest. In this work, we contribute to adebate about hypothetical sluggish diffusion phenomena
in high entropy alloys by investigating the vacancy migration behavior in CoCrFeMnNi high entropy alloys andtheir subsystems during the isochronal annealing after
electron-irradiation.

50

100 150 200 250 300 350 400 450

Annealing temperature (Υ)

Fig. 1 Mean positron lifetime in the electron-irradiated
CoCrFeMnNi, CoCrFe0.25MnNi, CoCrFeNi and CrFeNi
alloys after isochronal annealing.
5()(5(1&(6[1] C. Y. Hsu, J. W. Yeh, S. K. Chen and T. T. Shun,
Metall. Mater. Trans., $(2004), 1465.
[2] J. W. Yeh, S. K. Chen, S. J. Lin, J. Y. Gan, T. S. Chin,
T. T. Shun, C. H. Tsau and S. Y. Chang, Adv.Eng. Mater., (2004). 299.
[3] J. W. Yeh, Ann. Chim. Sci. Mat.,  (2006), 633.

̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿̿
31112

‑166‑

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,1752'8&7,21 In nuclear decommissioning ofFukushima Daiichi Nuclear Power Plant, observation of
the inside of the primary containment vessel (PCV) is oneof the key issues. For this purpose, many sensors including image sensor and radiation sensor have been underdevelopment [1, 2]. The data transfer from these devices
put into the PCV should be made by cable, because radio
wave cannot propagate out. The cable is also exposed to
the radiation field, and therefore some currents would be
induced by radiation. Such currents may cause an error in
the sensor output. Therefore, it is important to know how
large current would be induced at the cable, and to suppress the generation of the current. For this purpose, wehave observed the current induced at a coaxial cable bygamma-ray irradiation.
(;3(5,0(176 The gamma-ray irradiation was
performed at Co-60 gamma-ray irradiation facility at Institute for Integrated Radiation and Nuclear Science,
Kyoto University. The coaxial cable examined in thisstudy was 1.5D-QEV. A 15 m-long 1.5D-QEV cable waswound with a diameter of 20 cm. One end of the cable
was connected to a coaxial cable of RG58A/U, which had
been lain for taking the signal out of the irradiation room.
The measurements of the current were performed with acompact pico-ammeter. Another end of the cable wasterminated with a silicon diode installed in stainless steel
can equipped with the connector of the coaxial cable. Useof the silicon diode was because it has similar structurewith the solar cells, but it generates photocurrent only alittle. For comparison, measurements were done with thecable with the end open. For both cases, the outer shield
was grounded. Measurements were also made without
grounding the outer shield of the cable. The cable was set
at the position with different distance from the gamma-ray source. It was not easy to estimate the dose ofirradiation to the cable accurately, the results were arranged with the dose rate at the center of the wound cable; the practical dose rate would be lower than this value.
5(68/76 Figure 1 shows the results of the observed
currents as a function of the dose rate at the center of thewound cable. The data in Fig. 1 were acquired with thegrounded cable. When the one end of the cable was open,
approximately -40 pA was observed at the position where
the dose rate of irradiation was 200 Gy/h. When the end
was terminated by a silicon diode, the current increased
to about -110 pA at the same position. If the difference of
these results was attributed to the generation of photocurrent of the diode including radiation excited one, thecurrent should be shift towards positive. The reason forthe difference has not yet been clarified. The slope at thelower dose rate region is steeper than that at the higher
dose rate, and this would be attributed to the fact that theactual dose rate was lower than that at the center of thewound cable.
When the outer shield of the cable was not grounded,
the observed currents showed positive value in most cases. It was also shown that the observed current had agradual change. These phenomena would be due to thecharging of the cable. The present study showed the factthat grounding the outer shield of the cable is important
not only for the cancelling the electric noise but also forsuppressing the radiation effects.
$&.12:/('*(0(176 The present study was
supported by “Development of Dosimeter in Harsh Core
Radiation Environment”, through the Center of WorldIntelligence Project for Nuclear S&T and Human Resource Development by Japan Atomic Energy Agency.

400Current (pA)

Y. Gotoh, Y. Okuno1, N. Sato2, M. Imaizumi3,
T. Kobayashi4, M. Akiyoshi5, and T. Okamoto6

1.5D−QEV 15m
Open

−40
−80

1S1588+1.5D−QEV 15m

−120
−160
0

100
200
300
Dose rate at center (Gy/h)Fig. 1. Observed currents of the 1.5D-QEV cables
under the gamma-ray irradiation.

5()(5(1&(6[1] Y. Gotoh HWDO, IEEE Trans. ED  (2020) 1660-1665.
[2] T. Okamoto HW DO, “Development of Dosimeter inHarsh Core Radiation Environment”, Workshop on
Multicomponent Compounds and Solar Cells, Tokyo,
November 30 – December 1, 2018.

31118

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‑168‑

&2&RPSOH[6WUXFWXUHRI,RQV&RRUGLQDWHGZLWK+\GURSKLOLF3RO\PHU
,RQLF'LIIXVLRQLQ3RO\PHULF6WUXFWXUH8WLOL]HGE\3RO\LRGLGH,RQV  

A. Kawaguchi DQG Y. Morimoto,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21We have been investigating dynamical and interacted
structures between iodine (polyiodide ions, IQP-, P Q:
integer, Q > 1 ) and polymers.[1] While polyiodide ions( and their counter-ions, ex. K+ ion which presented
within I2-KI(aq) ) are prepared as solutes in aqueous solution, they can be diffused into various polymeric matrix
without softening nor melting. Such structures andprocedures are expected to introduce novel functionality
and wide applications to modify polymeric materials witheasy operation at R.T.[2]Or, ionic diffusion of polyiodide ions and their counterions from aqueous solution of polyiodides ("(1st) iodine
doping") can advance not only into hydrophilic polymers,such as polyamide-6 (PA6) or polyvinyl-alcohol (PVA),
but also into hydrophobic polymers, such as polyethylene(PE) or polyethylene-terephthalate (PET); polyiodide
ions in the aqueous solutions can easily diffuse even intoK\GURSKRELF matrices without melting.[3] Or, withinsome hydrophilic matrix, modification of structure (orientation of polymer chain, intercalated structure,,) can bealso observed.
Furthermore, posterior ionic diffusion on the previous
presence of polyiodides ("secondary doping") can also
advances for both hydrophilic polymers and hydrophobic
ones as ionic exchange process with the counter-ion previously introduced in "(1st) iodine doping". As phenomena, iodine-doped polymers can be regarded as"pseudo solvents" for ionic diffusion.[4,5] Inner precipitation of inorganic fillers can introduce hybrid composites without melting nor softening process for matrix
and, occasionally, can be applied for electrolessplating on hydrophobic surface with aqueous solution.
Such unexpected behaviors of polymeric structures inexistence of iodine (polyiodide ions) may be suggesting
contradictive effects: activated diffusive environments(softening, plasticization, disordering in matrix,) vs.
ordered structure (crystallization of crystalline polymer,
precipitation of inorganic fillers, modified orientation of
matrix).
On the other hand, structure of polyiodide ions can bealso modified vaguely; they are able to change molecular
structure and charge distribution not only in one moleculebut between the polyiodide ions, cooperatively and interactively. Therefore, interactive dynamics and structure
between polymers and iodine should be explained byextraordinary (also comprehensive and fundamental)
schemes specified for polymeric structure and polyiodide
ions.
',6&866,21
In the previously reported application utilizing "iodine
doping" and following "secondary doping", the resultsmean activation of ionic diffusion in inner space of pol-ymers. Characteristic and dynamic structure of the polyiodide ions show (almost general) affinity to both hydrophilic polymers and hydrophobic ones.
At first, we have to consider diffusion process of polyiodide ions into inner space of polymers, both for hydrophilic matrix and hydrophobic one while the polyiodide
ions (and counter-ions) are solutes in aqueous solutions.
Even though diameter of iodine atom is c.a. 4Å, they canbe spontaneously diffused in polymeric matrix at room
temperature; especially in some hydrophilic polymers(PA6, PVA,,), their diffusion is rapid and deep into thematrix. On the other hand, while iodine exist as
mono-iodide ion (I-) or tri-iodide ion (I3-) in each aqueous
solution for "(1st) iodine doping" process, polyiodide
ions doped and coordinated within polymers occasionallyexist as I3- or tetra-iodide ion, I5-. It means that iodine
elementally exists as polyiodide LRQV which have ioniccharge and that counter ions (K+, Na+, NH4+, ,,) also exist
simultaneously; they do not exist as "not-charged" molecules, such as methanol.
Secondly, polyiodide ions which are doped and exist at
inner space of polymeric matrix is QRW ones as moleculesin the aqueous solutions prepared on "iodine doping";
even if I3- molecules exist in deep region of the matrices,
they are QRW the similar molecules solved as the solutes inthe solution for "iodine doping". Or, it should be remarked that I5- which is occasionally observed in coordination with polymeric matrix is very minor components
in each aqueous solutions on "iodine doping"; I5- molecules are not diffused from the solutions but LQVLWX rearranged at inner space of matrix. It is not diffusion ofunchanged molecules but diffusion of the molecules
modified through diffusion. Since polyiodide ions caneasily change their molecular structure and charge distribution, they can be diffuse as different structure fromsolute in the aqueous solutions and as efficient form for
diffusion and binding. And it does not matter whether
the coordinated form or molecular structure is different
from the solutes in the doping solution or not. [to becontinued]$&.12:/('*0(176 These results are researchedwith Dr. Gotoh (Shinshu Univ.) and his staff and are partially funded by NEDO.[6]5()(5(1&(6>@ A. Kawaguchi, Polymer, , 3797-3798 (1994)
>@ patent. JPN-5444559 (2014).
>@ A. Kawaguchi, et.al., KURRI Prog.Rep.2015, 79-79.
(2016)
>@ $KDZDJXFKL et.al., SPring-8 User Exp. Rep.
(2000A), 354-354 (2000)
>@ A.Kawaguchi, Polym.Prep.Jpn., ,5116-5117(2013)
>@ “Projects for Practical Use from Innovation” sponsored by NEDO (2007-2009).

31122

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&2

A study on destruction of cesium aluminosilicate cageby gamma irradiation (1)H. Ohashi, R. TakakuDQG T. Saito1
Faculty of Symbiotic Systems Science, Fukushima University
1,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: Pollucite which is one of cesium
aluminosilicate com-pounds have attracted attention as a
final storage mate-rial of 137Cs. Pollucite is able to synthesized by hydro-thermal method in low temperature
below 300oC [1]. Pollucite has various properties thatfavor the immobilization of Cs ions.
However, the damage to the aluminosilicate frameworkby radiation decay is concerned because it contains 137Cs.
It has been reported that the effect of β-ray emission andnuclide conversion by β-decay of 137Cs on aluminosilicate framework is minor [2, 3]. On the other hand, there
are few reports of effects by gamma rays on pollucite
framework. Therefore, we examined the effect ofgam-ma radiation on the aluminosilicate framework of
Pollucite. Pollucite samples were synthesized to investigate the effect of gamma irradiation.

only single-phase pollucite. None of gamma irradiation
sample did not shifted diffraction peeks compared to before irradiation one. This indicated that there was nochange in the crystal structure of Pollucite.
Table 1 shows the various parameters obtained by theleaching test according to the PCT-A method, and thenormalized release rate (NRCs). In previous reports [5],the NRCs of Pollucite was around 10-5 to 10-6 [g m-2 d-1],
and was similar to the all samples after gamma irradiation
at this study. This indicated NRCs was not increased by
gamma irradiation.
From the above results, it was considered that the effectof gamma irradiation on the aluminosilicate frameworkof pollucite was not mostly observed until 100 kGy.

EXPERIMENTS: The solution was prepared at the Alconcentration of 50 mmol L-1 and the composition ratioof Cs5 Al1 Si2 O6 Na10 Cl11.2 K2 Ca0.2 (OH-)2.2 (H2O)220,
and placed in a Teflon inner cylinder pressure container.
Pollucite was synthesized by hydrothermal method,
holding the container at 180 oC for 72 hours. The resulting precipitate was washed. Thereafter, each solid wascollected by filtration and dried at 110 oC for 16 hours or
more.
The powder sample was divided into four, three of
which were gamma-irradiated at 1, 10, and 100 kGy.
Characterization was performed by XRD. The 7 days
leaching test by PCT-A method [4] was carried out toevaluate the change of Cs retention performance byframework damage. The normalized release rate, NRCs
[g m-2 d-1], was calculated by equation (1).

Fig.1. XRD patterns of (a) without irradiated, (b) 1 kGy,(c) 10 kGy, and (d)100 kGy irradiated sample.
Table 1.

Dose [kGy]
without-irr.
1
10
100



Where CCs [g L-1] was the concentration of Cs in thesolution, fCs was the weight ratio of the Cs in the sample
before leaching, SA [m2] was the sample surface area, V[L] was the volume of the leaching liquid, and t [day]was the test duration.
RESULTS: Figure 1 shows the XRD patterns of
Pollucite sample before and after gamma irradiation, andthe diffraction peak of Pollucite was indicated by theMiller index. All the patterns showed that they contained

Leaching test parameters in this study
fCs

SA V-1 [m2 L-1]

NRCs

0.35
0.35
0.35
0.35

134
141
141
141

1.510-4
1.510-4
1.210-4
1.310-4

REFERENCES:>@ Y. Yokomori et al., Sci. Rep., 4 (2014) 4195
>@ J. Fortner et al., Argonne National Laboratory,
Argonne, Illinois 60439 (2001).
>@ N. J. Hess et al., J. Nucl. Mater., 281 (2000) 22-33.
>@ ASTM C 1285-02 (2008).
>@ Z. Jing et al., J. Hazard. Mater., 306 (2016) 220–229.

31128

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&2 (IIHFWVRI%XIIHUVDQG6DOWVRQ1DQRVWUXFWXUHRI6R\EHDQ3URWHLQVDV5HYHDOHGE\6$;6
N. Sato, R. Urade, A. Okuda, K. Morishima, R. Inoue,and M. Sugiyama,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 It has long been known that soybeans contain abundant proteins. They consist of morethan 30% of dry matters of their seed. Thus, soybeans
have been eaten as nutritious natural food, not only as
unprocessed beans but also as soybean food products
such as WRIX and WRIX skin (\XED). 7RIX is a kind of hydrogels composed of soybean proteins, and accordingly
its property and quality are subject to coagulation behavior of soybean proteins. Aside from traditional soybean
food products like WRIX, soy protein isolate (SPI) havebeen industrially produced and provided to the commercial market in recent years for improving physical property of various food products by adding them to thosefoods. Soybean proteins are also used for making mimicmeat products for vegetarians and vegans. World-wide
increase in health consciousness leads to growing importance of soybean protein usage. From these reasons,soybean proteins are one of key substances in the field offood science.
In order to obtain high-quality soybean food products
or SPI-containing foods, it is necessary to deeply understand the structure of soybean proteins at the molecularlevel. In particular, structural changes induced by thevarious conditions such as temperature change, salt addition and coagulant addition are of great significance toelucidate the relationship between the structure of proteins and the physical property of foods containing soybean proteins. For structural analysis on opaque, disorderand condensed soft matters such as gels, colloids, andrubber, small-angle X-ray and neutron scattering (SAXS,SANS) has been proved to be a useful technique, and it isalso expected to be effective for structural analysis offoods, which has similar features to above soft matters.
Therefore we have been studying the nanostructure ofwheat and soybean proteins by SAXS and SANS. The
behavior of isolated and aggregated protein molecules inaqueous solutions and hydrates has been investigated bytaking advantage of SAXS and SANS.
In this study, we conducted a SAXS analysis on two
major soybean proteins, β-conglycinin and glycinin,
which have been conventionally referred to as 7S and
11S, respectively, according to their sedimentation coefficients determined by analytical ultracentrifugation. Difference of nanostructure of 7S and 11S in pure water andbuffer solutions was examined by SAXS. Effects of NaCl
addition was also investigated.
(;3(5,0(176 Soybean proteins 7S and 11S wereextracted from hexane-defatted powder of soybean cultivar “Enrei” under a reducing condition with
2-mercaptoethanol. Isoelectric precipitation was applied)LJ  SAXS profiles for 7S (left) and 11S (right) in
0.5% pure water and KPi buffer solutions.
to isolation of each protein. By adjusting pH of the extract solutions, 11S and 7S was precipitated at pH 5.8 andpH 4.5, respectively. SAXS measurements were performed with a laboratory SAXS instrument (NANOPIX,
Rigaku) installed at Institute for Integrated Radiation and
Nuclear Science, Kyoto University. Each protein dissolved in pure water or 35-mM potassium phosphate(KPi) buffer solutions at pH 7.5 in presence of 0 or 0.8 M
NaCl was put into aluminum cells and set for SAXS
measurements. The wavelength of X-ray was 1.54 Å, thesample-to-detector distance was 1300 mm and the available T-range was 0.08 – 2.2 nm-1. Model calculation of
SAXS profiles from crystal structure was done with asoftware, CRYSOL [1].
5(68/76 Fig. 1 shows SAXS profiles measured for
0.5% 7S and 11S solutions at 25°C. A small peak appeared around 1.2 nm-1 in KPi buffer solutions, which isan indication of trimer ring structure consisting of threesubunits. In pure water, however, this peak was not recognizable, suggesting that the subunits cannot form trimer ring structure and exist as monomers in pure water.
When 0.8 M NaCl was added to the KPi solution of 7S,
the peak at 1.2 nm-1 became weaker and the shoulder at
0.4 nm-1 shifted to higher-T. However, such changes were
not observed for 11S. These profiles agree with the model
calculation results for crystal structure of monomer, trimer and hexamer. Therefore it was demonstrated thatmonomeric subunits in pure water are assembled into
hexamers in KPi buffer solutions by stacking two ring
trimers, and dissociated into trimers at higher ionicstrength conditions only for 7S.
5()(5(1&(6[1] D.I. Svergun HWDO, -$SSO&U\VW, (1995) 768.

31137

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&2

3RURVLW\0HDVXUHPHQWVRI6LQWHUHG6LOYHU%RQGLQJ3ODWHV

K. Wakamoto, T. Otsuka, K. Nakahara, A. Yabuuchi
and A. Kinomura
3RZHU'HYLFH5 ''HSDUWPHQW52+0&R/WG,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\digital circuits. Total counts for each measurement wereapproximately 106 counts.

,1752'8&7,21  Sintered silver has attracted muchattention as a die-attach material for the power electronics, owing to its high heat dissipation capability [1]. On
the other hand, the coefficient of thermal expansion(CTE) inevitably does not match each other of the materials used in a power system. Thus the heat-cycle oriented
mechanical stresses deteriorate die-attach materials, andtherefore the mechanical properties of sintered silver impinge on the reliability of electricity systems.
However, nobody can predict how long sintered silver
sustains, because the material is porous and its mechanical properties heavily depends how porous it is. Accordingly, the research is highly demanded to measure theporosity.
The porosity rate (S) of sintered silver is reported bysome papers [2-3], where S is measured by using crosssectional scanning electron microscopy (SEM). Thesestudies focus only estimates the μm-order pores of sintered silver materials, not nm-order pores such as crystalline defects. Positron lifetime measurement method has
advantages for this purpose. To this end, therefore, theauthors used a conventional positron annihilation lifetime
spectrometer in Kyoto University to estimate the
nm-order pore sizes embedded in sintered silver withvarious S·s by measuring the positron lifetime of the material.
(;3(5,0(176 The fabrication process of sintered
silver films is described as follows. Paste including
silver nm-particles was stencil printed on a metal plate,
and the containing organic solvent was dried at 140ºC for
1 h. These dried films were sintered at 300 ºC for 10 min
with uniaxial press via a carbon buffer sheet with 0.5 –120 MPa pressure. The film shape was 5 mm square and50-μm thick. Positron annihilation lifetime spectroscopy
was performed to evaluate bulk lifetimes of the samples
by using a 22Na source sealed with 12.5 μm Kapton foils.
The thickness of the samples was approximately 50 μm.
Four sample plates were stacked and measured together
to stop all the positrons from the source inside the sample.
The measure samples are summarized in Table,

5(68/76 The data from the 1st sample set to investigate pressure dependence was analyzed as follows.
Measured lifetime spectra were decomposed into threecomponents as shown in Fig. 1. The lifetimes and intensities of the first and third components changed depending on formation pressure, while the second lifetime
and intensity were almost constant except for the lowest
pressure sample. In fig. 1(a), average lifetimes calculated from lifetime and intensity values were plotted aswell. The average lifetimes were almost constant for all
the samples. The lifetime values obtained from a literature for bulk Ag and monovacancy in Ag were indicatedwith broken lines in fig. 1(a). The second and third lifetime components can be attributed to monovacancies andvacancy clusters. It is necessary to further investigate
the origin of each lifetime components to know the behavior of nanometer-sized voids (vacancies) that cannot
be detected in secondary electron microscopy.
6800$5<Porosity of sintered Ag plates was characterized as a function of formation pressure by conventional positron annihilation lifetime spectroscopy. The
third lifetimes corresponding to vacancy clusters changed
depending on formation pressure, while the average lifetime was almost constant.

7DEOH, Summary of the measured specimens.
6DPSOH
A
B
C
D

6LQWHULQJWHPS
R&

3UHVVXUH
03D 

6DPSOHVL]H

300

120
80
30
0.5

5mm squareand200-μmthick

Fig. 1 Lifetimes and their intensities of the samples.

The spectrometer consists of two scintillation gamma-ray
detectors with BF2 crystals and a spectrometer based on

5()(5(1&(6[1] KIM S. SIOW, Journal of ELECTRONIC MATERIALS.,  (2014) 947-961.
[2] T. Yousseff HW DO., Microelectronics Reliability., (2015) 1997-2002.
[3] M. Takesue HWDO., Proc. PCIM.,(2018) 148.

31143
‑172‑

&2 'LIIHUHQFHV LQ WKH 5HFRYHU\ %HKDYLRU RI (OHFWURQ,UUDGLDWLRQ,QGXFHG 9DFDQFLHV LQ
0HWDOVZLWK'LIIHUHQW3XULWLHV
A. Yabuuchi, M. Tanaka, and A. Kinomura,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Since tungsten (W) is expected asa plasma-facing material for fusion reactors, many studies on vacancy-type defects in W are carried out using
positron annihilation spectroscopy. Based on several
first-principles calculations, the positron lifetime ofmonovacancy in W is expected to be 193−200 ps. On theother hand, defects having positron lifetimes of165−180 ps have been observed in electron-irradiated W.
In this study, the annealing behaviors of electron-irradiation-induced vacancies in two kinds of W
samples with different purities were observed by using a
positron annihilation lifetime spectroscopy in order tounderstand the cause of the difference between the calculated and experimental values. In addition, positron lifetimes in vacancy-impurity complexes consisting of several possible impurity atoms were also calculated andcompared with experimental values.
(;3(5,0(176 Well annealed W samples having
purities of 99.999% (5N) or 99.9% (3N) were irradiatedwith 8-MeV-electrons to a total dose of 5×1019 e−/cm2.
The sample temperature was kept at about 373 K during
the irradiation. The irradiated samples were isochronallyannealed at 50 K steps with a duration of 15 min. Aftereach annealing, positron annihilation lifetime measurements were performed at room temperature. The acquired
positron annihilation lifetime spectra were decomposed
into two components. The longer lifetime component wasrecognized as the component derived from the irradiation-induced vacancies.

Fig. 1. Defect-related positron lifetimes τ2 and theirintensities ,2 for 5N- (open circles) and 3N-W (open
pentagons) samples as a function of annealing temperature. Calculated positron lifetime for isolated monovacancy (195 ps) is also depicted as a dashed line.

5(68/76 Figure 1 shows the changes in the longer
positron lifetimes and their intensities of both samples
during isochronal annealing [1]. The positron lifetimes ofboth as-irradiated samples (~170 ps) are about 25 ps
shorter than the calculated positron lifetime of isolatedmonovacancy (195 ps). This implies that the vacancies
introduced into W by electron-irradiation does not exist
as isolated monovacancies, but rather exist as vacancy-impurity complexes. The positron lifetime calculations
revealed that the positron lifetime becomes shortened
from 195 ps to ~170 ps when a monovacancy binds withinterstitial-type impurity atoms such as carbon, oxygen,and nitrogen. It was also found that the positron lifetimeof vacancy-hydrogen complex becomes only shortened to
185 ps, whereas it becomes shortened to ~170 ps when
two hydrogen atoms are bound to a monovacancy.
5()(5(1&([1] M. Tanaka, A. Yabuuchi, and A. Kinomura, AIP Conf.
Proc.,  (2019) 050014-1−050014-4.

Fig. 2. Calculated positron density distributions at(a) isolated monovacancy, (b) vacancy-carbon complex, and (c) vacancy-iron complex. The atomic positions are also depicted as spheres.

31157

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&2

'LIIHUHQFHV LQ WKH 'HYHORSPHQW RI 9DFDQF\7\SH 'HIHFWV 'XULQJ $QQHDOLQJ ZLWK'LIIHUHQW,UUDGLDWHG,RQ6SHFLHV

A. Yabuuchi, M. Tanaka, and A. Kinomura

5()(5(1&(6[1] S. Mantl and W. Triftshäuser, Phys. Rev. Lett., (1975) 1554−1557.
[2] A. Yabuuchi, M. Tanaka, and A. Kinomura, J. Nucl.
Mater.  (2020) 152018-1−152018-5.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Since tungsten (W) is expected touse as a plasma-facing material for fusion reactors, theeffects of hydrogen (H) and/or helium (He) ion irradiation into W have been well studied. Recently, several
studies are carried out to reduce the heat load on W wallby injecting neon (Ne) or argon (Ar) gas into the fusion
plasma. Positron annihilation spectroscopy is a useful
tool for characterizing vacancy-type defects in materials.
Thus, several positron-based studies of defects in H+- or
He+-irradiated W have been reported. However, few
studies have investigated the defects in Ne+- and/or
Ar+-irradiated W by using positrons. Irradiating heavier
ions than H+ and/or He+ may cause more serious damage
to W. In this study, He+- and Ne+-irradiated W samples
were prepared and investigated the differences in the developmental process of irradiation-induced defects during
annealing by using a slow positron beam.
(;3(5,0(176 The well annealed W samples were
irradiated with He+ or Ne+ ions with an energy of 50 keV.
The irradiated and unirradiated samples were probed by aslow positron beam to acquire the Doppler broadening of
the annihilation radiation (DBAR) spectra. The DBAR
spectra were characterized by an 6-parameter which represents the proportion of annihilation events with a small
Doppler shift, and a :-parameter which represents the
proportion of annihilation events with a large Doppler
shift. In addition, 5-parameters were also derived fromthe 6- and :-parameters [1]. The 6- and :-parameters
depend on both defect species (defect size) and defectconcentration, while the 5-parameter does not depend on
the defect concentration but only on the defect species.
5(68/76 Figure 1 shows the annealing temperaturedependence of 6-parameters for both irradiated samples.
The increased 6-parameters of as-irradiated both samples
are finally reduced to the almost unirradiated-state byannealing at 900°C. Judging from the changes in
6-parameters, superficially, the irradiation-induced defects appear to have been recovered in both samples.
However, the changes in 5-parameters shown in Fig. 2
indicate that the developmental processes of irradiation-induced defects in both samples are different during
annealing. Figure 2 shows that defect species in the
He+-irradiated W finally become the same as those in theunirradiated W (LH, the irradiation-induced vacancies are
fully recovered). In contrast, the changes in 6-, :-, and5-parameters during annealing indicate that irradiation-induced vacancies aggregate and grow into larger
vacancy clusters in Ne+-irradiated W [2].

Fig. 1. 6-parameters as a function of annealing temperature obtained from He+- and Ne+-irradiated tungsten. All the 6-parameters are normalized to that obtained from unirradiated tungsten probed with positronenergy of 20 keV. The He+- and Ne+-irradiated tungsten were probed with positron energies of 8.5 keV and6 keV, respectively. 6-parameters obtained from theunirradiated tungsten probed with positron energies of
6 keV and 8 keV are also depicted as dashed lines.

Fig. 2. 5-parameters as a function of annealing temperature obtained from He+-and Ne+-irradiated tungsten. All the 5-parameters are derived from the normalized 6- and :-parameters. The 5-parameter obtained from unirradiated tungsten probed with positronenergy of 1 keV, corresponding to positron annihilation
at the surface, is also depicted as a dashed line.

31158

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3UREHGE\D6ORZ3RVLWURQ%HDP

T. Ozaki, H. Sakane1, T. Kashiwabara, A. Yabuuchi2 andA. Kinomura2
6FKRRORI6FLHQFHDQG7HFKQRORJ\.ZDQVHL*DNXLQ8QL
YHUVLW\
6+,$7(;&R/WG,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Superconducting materials, suchas GdBa2Cu3O7íį (GdBCO) investigated in this work, are
known to improve a high magnetic field resistance byforming lattice defects using ion-irradiation techniques.
The Doppler broadening of annihilation radiation(DBAR) spectra become sharpened by annihilating positrons at vacancy-type defects, which enables us to characterize the concentration and/or size of vacancy-type
defects [1]. In this work, tape-shaped GdBCO films irradiated with 2-MeV-Au2+ or 10-MeV-Au4+ ions wereprobed by a slow positron beam.

Fig. 1.

6 parameters for unirradiated GdBCO tape.

(;3(5,0(176 The GdBCO(500 nm)/CeO2(150 nm)/Y2O3(150 nm)/Ni/Cu/SUS samples were irradiated with
2-MeV-Au2+ (4×1012 Au2+/cm2) or 10-MeV-Au4+ (6×1012
Au4+/cm2) ions. The 2 MeV and 10 MeV ions stop in the
GdBCO film and penetrate the GdBCO film, respectively.
The unirradiated and irradiated samples were probed by
the KUR slow positron beam and the DBAR spectra wereacquired. The sharpness of the DBAR spectra is evaluated by a value called the S parameter, which becomesgenerally lower when positrons annihilate in a perfectlattice, and higher when positrons are trapped into vacancies [1].
5(68/76 Figure 1 shows S parameters for the unirradiated sample as a function of incident positron energy.
The S parameters in the energy region of 5í12 keV correspond to positron annihilation in the GdBCO film. Figures 2 and 3 show S parameters for the 2-MeV-Au2+- and10-MeV-Au4+-irradiated samples. Contrary to our initialexpectation, both irradiated samples show a reduction in
S parameters compared to the unirradiated one. This reduction in S parameters implies that the unirradiatedsample already contained vacancy clusters larger than
irradiation-induced vacancies. When a large number ofrelatively small vacancies are formed by ion irradiation,
most positrons are trapped at the irradiation-induced vacancies rather than the pre-existing vacancy clusters. Positrons annihilated in small vacancies bring smaller S parameters than positrons annihilated in vacancy clusters,
and thus the reduction in S parameters was considered tobe caused by ion irradiation.
5()(5(1&([1] R. W. Siegel, Ann. Rev. Mater. Sci., 10 (1980)
393í425.

Fig. 2.
6 parameters for 2-MeV-Au2+-irradiated
GdBCO tape with a total dose of 4×1012 Au2+/cm2.

Fig. 3.
6 parameters for 10-MeV-Au4+-irradiated
GdBCO tape with a total dose of 6×1012 Au4+/cm2.

31159

‑175‑

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irradiation effects on optical elements and piezo-actuators
used in ITER. Expected 1 MeV Silicon equivalent fluenceis -  n/c5 depending on locations of components.
In order to investigate the effect of such high fluence on
the actual components in a short time, neutron irradiation
was performed using the slant exposure tube and the pneumatic tubes of the KUR. Although there are similar studies
in Europe [2], they don’t cover all the components necessary for ITER plasma diagnostic systems developed by Japan. #01:9-879;5)164@89-:-6;:-..-+;7.6-<;976199),1)
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9ROFDQLFDQG7HFWRQLF+LVWRU\RI3KLOLSSLQH6HD3ODWH 6RXWKRI-DSDQ 
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O. Ishizuka, S. Sekimoto1, R. Okumura1, H. Yoshinaga1,
Y. Iinuma1 DQGT. Fujii2*HRORJLFDO6XUYH\RI-DSDQ$,6DQG7,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ2VDND8QLYHUVLW\,1752'8&7,21 Submarine volcanic rocks are
known to give ages different from their true eruption ages
in some cases. This is due to the existence of excess 40Ar
in the rapidly quenched glass or Ar loss and K remobilization caused by reaction with seawater or hydrothermal fluids. Stepwise-heating analysis in 40Ar/39Ar dating is particularly useful for dating submarine volcanics.
Robust tectonic reconstruction of the evolving Philippine Sea Plate for the period immediately before and after
subduction initiation at ~52 Ma to form the Izu-BoninMariana (IBM) arc is prerequisite to understand cause of
subduction initiation (SI) and test competing hypotheses
for SI such as spontaneous or induced nucleation. Understanding of nature and origin of overriding and subducting
plates is especially important because plate density is a key
parameter controlling SI based on numerical modeling(e.g., Leng and Gurnis 2015). There is increasing evidence
that multiple geological events related to changing stressfields took place in and around Philippine Sea plate about
the time of SI ~52 Ma (Ishizuka et al., 2011). For our understanding of the early IBM arc system to increase, it isimportant to understand the pattern and tempo of these geological events, particularly the duration and extent of seafloor spreading in the proto arc associated with SI, and its
temporal relationship with spreading in the West Philippine Basin (WPB).
The YK19-07S cruise aimed to investigate origin and age
of formation of ocean basins in and around the Daito Ridge
group. Especially ocean basins which potentially existed
in the period of SI to form the IBM arc were the major
targets of this cruise, because ocean crust of these basinsmight be part of overriding plate when subduction of Pacific plate initiated to form IBM arc. Since gravitational
instability between the neighboring plates is supposed to
be a critical factor for subduction initiation, it is importantto understand characteristics (age, origin, crustal structure)of overriding plate to test hypotheses of subduction initiation. Recovery and characterization of igneous crust ofthese basins will provide crucial information about thepossible basement of the IBM arc and critical constraints
to evaluate models for subduction initiation along the Pacific margin. Recent cruises in the Philippine Sea basins
recovered basalts from ocean crust along the major tectonic lines such as the Oki-Daito Escarpment and Mindanao Fracture Zone of the West Philippine Basin. Thesesamples were dated by 40Ar/39Ar dating method to obtainage of formation of the basins.

(;3(5,0(176 Samples were wrapped in an aluminum foil packet and the packets were piled up in a purealuminum (99.5% Al) irradiation capsule (9 mm diameterand 30 mm long). The irradiation capsule was partitioned
into 3 compartments to minimize the horizontal flux variation across the capsule.
For the experiments described here, around 5 mg of sample was analysed. Only minimum acid leaching was applied to the glass samples, i.e., ultrasonic cleaning with 3M
HCl for 10 minutes at room temperature. After this acidtreatment, the glass chips were examined under binocular
microscope before packed for irradiation.
5(68/76 40Ar/39Ar dating of fresh basalt glasses from
YK19-07 cruise returned variable results, with some “disturbed” age spectrum (Fig. 1). This spectrum is characterised by some steps with irregularly older ages among thosewith relatively constant ages of around 58 Ma. These older
steps, however, show consistent Ca/K ratios with othersteps. This strongly implies that these steps are not associates with particular minerals or melt inclusion, but possibly represent degassing from bubbles or “gas pockets”
which partially preserve mantle-derived Ar. Konrad et al.
(2019) reported similar spectrum from stepwise heating
analysis of pyroxene crystals.
Presence of Ar inherited from mantle is a critical problem
in dating glass samples. We still need more examples ofhigh-precision dating experiments to understand behaviorof mantle-derived Ar and its effect on age spectrum.

Fig. 1 Age spectrum for the basalt glass from the northernmost
West Philippine Basin recovered by submersible Shinkai 6500.

5()(5(1&(6[1] O. Ishizuka et al. , Earth Planet. Sci. Lett., 306 (2011)229-240.

31012

‑177‑

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002>2>!         1&5@04A>!              =    ! = ?                    !       @ 3B                # #  ) +  ,  "                @3B 607   #      !                             "          # + ,   "                                                            * $#                       %<0302103$0 $/023<10&0& "  * 3#      #(# )* +, "        "  $%%5130$/        !             =?

2$03&
‑178‑

&2

Ar-Ar dating of submarine basalts

N. Hirano, H. Sumino1DQG S. Sekimoto2
Center for Northeast Asian Studies, Tohoku University
1
Graduate School of Arts and Sciences, University ofTokyo
2,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION:
On the western part of the
Pacific Plate, most seamounts formed during theCretaceous pe-riod in the so-called West PacificSeamount Province (WPSP). The eustatic sea level andglobal average tem-perature, increasing seafloor
spreading rate, and volumi-nous
volcanic
activities
occurred
duringthe mid-Cretaceous period. Manyof seamount chains, how-ever, cannot be explained by
the classical hotspot and mantle plume hypothesis as
well as the Hawaii-Emperor Seamount Chain could be
done. Many of seamount and knoll had left their dating
behind the volcanic evolutions on the western PacificPlate. Moreover, the lithospheric flexure-induced
volcanoes (petit-spots) are recently de-scribed at theouter-rises of Japan Trench prior to the subduction ofnorthwestern and the western Pacific Plate [1]. Nobody
has found such intra-plate volcanoes pre-ceded by thepetit-spot volcanic activities since younger WPSP
hotspots during Late Cretaceous on the western PacificPlate. Similar volcanoes have been reported at
subduction zones worldwide (e.g., the Japan, Tonga,
Chile, and Java trenches) [1][2][3][4][5]. We, therefore,
conduct to determine the eruption ages of volcano using
Ar-Ar dating to understand the evolution of pacific Plate
during Cretaceous to present.
EXPERIMENTS: The research cruise using R/V Yokosuka equipped with the submersible SHINKAI 6500,
was conducted around the Marcus Island on May 2010 inorder to know the detail history during the formation of
the Marcus Island (Fig. 1). Radiometric Ar-Ar dating iscommonly used to determine the ages of submarine lavas
obtained during the submersible dives, because the traditional K-Ar dating is impossible to remove the alteration
part of rocks [6]. After the rock-samples, crushed to100-500 μm grains, they were irradiated by neutrons in areactor to produce 39Ar from 39K during a few hours.
During the irradiation, samples were packed with EB-1
biotite flux monitors [7], K2SO4 and CaF2 as correcting
factors in an aluminum capsule. Then, radiogenic 40Ar,
daughter nuclide of radioactive 40K and parent, 39Ar instead of 40K, were simultaneously analyzed using a massspectrometer with an extraction technique of mul-ti-stepheating of approximately every 50 to 100 °C be-tween
500 to 1500 °C.
RESULTS: We obtained an estimated eruption ageof no more than 3 Ma base on several dating methodsof Ar-Ar and others. The NW Pacific petit-spots andthis newly described WPSP petit-spot were all erupted
from locations in the zone of concave flexure on theouter rise of the lithosphere, prior to its subduction at a
trench.

7KH WPSP eruption site is >1100 km from theOgasawara Trench and 800 km from the Mariana Trench.
These relatively large distances from the trench axes
could possibly be explained by the wider outer rise inthis subduction system, where the distance to the crest of
the outer rise at the Mariana Trench is greater than inother subduction systems [8].
36˚N

32˚N

WPSP

28˚N

24˚N

20˚N

Water depth (m)140˚E-1000025˚ 00'

-8000

144˚E
-6000

148˚E
-4000

-8000

Minamitori shima(Marcus) Island

152˚E

-2000

0

-6000

156˚E
2000

-4000

-2000

4000

Water depth (m)
50 km

0

Tomoda Seamount24˚ 30'24˚ 00'23˚ 30'

Takuyo-Daigo
Seamount23˚ 00'153˚ 30'154˚ 00'154˚ 30'155˚ 00'

Fig. 1. Bathymetric map of the study area. Yellow
box on the upper figure indicate the area of map
shown in lower figure. The red square on lower figure
indicates the area discovered the young volcano.
REFERENCES:>@ N. Hirano et al., Science, 313 (2006) 1426-1428.
>@ N. Hirano et al., Basin Res., 20 (2008) 543-553.
>@ N. Hirano et al., Geochem. J., 47 (2013) 249-257.
>@ R. Taneja et al., Gondwana Res., 28 (2014) 391–406.
>@ N. Hirano et al., Marine Geol., 373 (2016) 39–48.
>@ I. McDougall and T. M. Harrison, in Geochronology
and Thermochronology by the 40Ar/39Ar Method,(Oxford, New York, 1988).
>@ N. Iwata, Ph.D. Thesis, Tokyo Univ. (1998).
>@ N. Hirano et al., Deep-Sea Re. I, 154 103142 (2019).

31039

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&2

5HFU\VWDOOL]DWLRQRIDQDPRUSKRXV6LOD\HUE\+LRQEHDPDQGHOHFWURQEHDPLUUDGLDWLRQJ. Nakata, T. Iha, Y. Hoshino, A. YabuuchiDQG A. Ki
nomuraJ.Nakata1, T. Iha1, Y. Hoshino1, A. Yabuuchi2, A. Kinomura.2'HSDUWPHQWRI0DWK3K\V.DQDJDZD8QLYHUVLW\'HSDUWPHQWRI0DWK3K\V.DQDJDZD8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH

5HVHDUFK5HDFWRU,QVWLWXWH.\RWR8QLYHUVLW\.\RWR8QLYHUVLW\,1752'8&7,21  IBIEC (ion beam induced epitaxial crystallization) phenomena have been widely studied for about forty years, especially by using MeV ion
beam irradiation.1-3) The author proposed mechanism of
IBIEC, consisting of formation of vacant spaces in theamorphous Si (a-Si) layer after vacancy-interstitial recombination in the crystalline Si (c-Si) substrate. The
finally remained vacancies after recombination produced
at the a-c interface were supplied to the amorphous layer
and became vacant spaces in it. These resulted in the vibrational motion of Si atoms wider and more freely,
eventually epitaxial recrystallization occurred at lower
temperature than that in normal heat treatment. Electronhole pairs creation also occurred effectively due to MeV
ion irradiation. When they are recombined, emitted radiation energy also enhanced the vacancy or interstitial migration, eventually recrystallization rate was greatly enhanced.4) However, the role of inelastic electronic scattering in the IBIEC process has not been necessarily anddirectly proved. Thus, we tried to make sure the effect ofelectronic scattering in the IBIEC process. We compared
the IBIEC rate by H+ ion beam with the EBIEC (Electron
Induced Epitaxial Crystallization) rate by e-beam.
(;3(5,0(176 190 keV Si+ ions were implanted at50~60Υ with doses of 5, 10, 20, 50, 100×1014/cm2 for
10 μA beam current, to form damaged and a-Si layers in
the c-Si substrates. Then, 1) IBIEC, 2) EBIEC, 3) furnaceannealing were undergone to these above obtained damaged and amorphized substrates. The H+-IBIEC wasconducted at 150 keV with 2×1016 cm 2 doses for ~3 μA
continuous beam current at 400Υ for 23 hours. 2) The
EBIEC was conducted at 7.2 MeV with 4.07×1019/cm2
doses for ~70 μA pulsed electron beam at 400Υ for 46
hours. 3) thermal annealing for the as-amorphized sample
was conducted at 400Υ for 23 hours in vacuum chamber,and for 46 hours in the gold-furnace during Ar ambient
flowing. The thicknesses of a-Si layers of these threesamples were measured by the Rutherford Backscattering
method with 2 MeV Li2+ ions, SSB detector being settled
at 120Υ angle to the Li2+ beam direction.
5(68/76 Figure 1 and 2 show respectively the RBS
spectra after IBIEC (markࠐ in Fig. 1) and EBIEC (markࠐ in Fig. 2) to the amorphized samples with 2.0×1015/cm2 Si doses. We also show in these figures for the
as-implanted and annealed samples at 400Υ for 23hours (mark‫ ڸ‬in Fig. 1) and at 400Υ for 46 hours(mark‫ ۂ‬in Fig. 2). As clearly seen in Fig. 1, IBIEC at400Υ sample (markࠐ) was crystallized sharply, compared with that (mark‫ )ڸ‬of the 400Υ-annealing one invacuum for 23 hours.

)LJ5%6VSHFWUDIRUWKH,%,(&VDPSOH

)LJ5%6VSHFWUDIRUWKH(%,(&VDPSOHAs also clearly seen in Fig. 2, EBIEC sample at 400Υ
(markࠐ) was not entirely crystallized at all, comparedwith that (mark‫ )ۂ‬for the furnace-annealed one in Ar
ambient at 400Υ for 46 hours.
',6&866,216: In calculation, displaced Si atom density is almost the same for both 150-keV H+ ion for 2×
1016 cm 2 and 7.2-MeV electron for 4.07×1019/cm2 doses
at around the a-c interface region. Furthermore, considering the total doses of H+ ions and electrons, total inelastic electronic deposited energy density in EBIEC is about
only 8 times higher than that in IBIEC in spite of the2000 times higher doses in EBIEC. Consequently, it
seems that the IBIEC rate is mainly determined by theelastic energy deposition and it cannot be decisively concluded that the electronic deposited energy density enhances the crystallization rate. It should be noted that
IBIEC rate generally decreases as the irradiation dose
rate increases. Thus, we should thoroughly compare thedose rate of EBIEC by SXOVHG electron beam with thedose rate of IBIEC by FRQWLQXRXV H+ ion beam.
5()(5(1&(6 J Nakata and K Kajiyama: Appl.Phys.Lett.(8)(1982) 686-688.
 J Nakata and K Kajiyama: Jpn. J. Appl.Phys.,
(1982) 211-216.
 J Nakata: Phys. Rev. %(1991) 14643-14668.
 J Nakata: J. Appl. Phys. (1996) 682-698.

31049

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&2 Study on Elemental Concentration in the Atmospheric Particulate Matter by INAA
N. Hagura1, 2, Y. Okada2, H. Matsuura1, 2, T. Uchiyama2

KUR. And long and medium-lived nuclides, after coolingfor one or two weeks, transported to the TCU-AERL, andwas measured by a HP-Ge semiconductor detector. JLk-1
was used as a comparative standard substance.

Nuclear Safety Engineering, Tokyo City University
Atomic Energy Research Laboratory, Tokyo City University

2

INTRODUCTION: The Atomic Energy Research Laboratory of Tokyo City University (TCU-AERL) has operated the research reactor "Musashi Institute of Technology Research Reactor (MITRR)" from 1963 to 1989,
and has performed various neutron experimental researchthat is including instrumental neutron activation analysis(INAA). In 2003, it officially decided to decommission
the research reactor, and it is currently in the decommissioning stage. At present, all the fuel has been carried out,
and it is in the phase of storing and managing radioactive
compounds.
Since 2002, sampling of airborne particulate matter havebeen performed on our facility. Even before that, researchon the measurement of radioactivity in the environmenthas been conducted mainly by Dr. Honda, deceased in2014, and the concentration distribution of Be-7 andPb-210 and chemical form in deposition have been analyzed [1]. These studies mainly focused on the behaviors
of yellow sand that came to the Japanese archipelago.
After the accident in Fukushima in March 2011, studies
on the dynamics of radioactive cesium have been conducted. Especially, focusing on the difference between
the rapid decay of radioactive cesium concentration after
the accident and the gradual decay after several months,
we have been investigating the relationship between the
different chemical forms [2, 3].
The sampled filters have been accumulated in the laboratory and are ready to be analyzed again. This fiscal year,
we aimed to detect the elements other than cesium byneutron activation analysis, targeting the samples fromFebruary to July in 2011.

RESULTS: Figure 1 shows the time-series distributionof elements for each sample. Figure 2 shows the correlation coefficients of these 10 nuclides. As expected, we
obtained reasonable results of relatively high concentrations of Na, Al, Ca, and Fe. Regarding the correlation
coefficient, it was shown that Al and Ca are relatively
strongly correlated with other elements.
In the future, we plan to proceed with the analysis of alarge number of samples in combination with the PIXE
analysis method using the tandem accelerator at our facility (TCU-Tandem) [4], because it is impractical to analyze
all samples by the INAA method.
Table 1. Irradiation conditions
Irradiationdate
2019/10/1
2019/10/23

time
position
30 sec Pn-3
60 min Pn-2

2019/12/3

30 secPn-3

Operating
Thermal neutron flux
power
12
2
4.7 x 10 n/cm /sec
122
5.5 x 10 n/cm /sec
1 MW
12
2
4.7 x 10 n/cm /sec

2020/1/15

60 min Pn-2

5.5 x 10 n/cm /sec

31052

‑㻝㻤㻝‑

Al

Ca

Sc

Ti

V

Cr

2

Mn

Fe

Ce

1.0E+03
1.0E+02
1.0E+01
1.0E+00
1.0E-01

2011/2/8 2011/2/15 2011/2/22 2011/3/2 2011/3/10 2011/4/23 2011/4/29 2011/5/14 2011/5/21 2011/6/3 2011/6/11 2011/6/30 2011/7/8 2011/7/13
11F208

11F215

11F222

11F302

11F31011F423

11F429

11F514

11F521

11F603

11F611

11F63011F708

11F713Fig. 1. Transition of element concentration for each sample from February to July in 2011
1D

EXPERIMENTS: We use a high volume air sampler(Shibata Scientific Technology LTD., HV-1000F, filter:
ADVANTEC, QR-100 (collection efficiency: 99.99% for
0.3 ȝm particles)) with an inhalation flow rate of 700 L
min-1. Samples are collected approximately every week.
The radioactivity of the filter that has collected dust ismeasured by a high-purity germanium semiconductor
detector (ORTEC, GMX-15190-P, wide range energy
type, relative counting efficiency: 20.1%, FWHM:
1.22keV at 122keV, 1.9keV at 1.33MeV, wave height
discriminator: SEIKO EG&G, MCA-7700), and a part of
the filter was stored for neutron activation analysis.
Irradiation was performed at the research reactor KUR at
the Institute for Integrated Radiation and Nuclear Science,
Kyoto University, between the October and January withfour machine times in FY2019. The irradiation conditions
are shown in Table 1. The measurement of radioactivityof short half-life nuclides was carried out using the
HP-Ge semiconductor detector of the hot laboratory ofNa

1.0E+04

12

ng/m3

1

1D

$O

&D

6F

7L

9

&U

0Q

)H

&H
Uˀ

$O&D

!Uˀ

6F
7L

!Uˀ

9&U

!Uˀ

0Q)H

!U&H

Fig. 2. Distribution chart of correlation coefficient between elements
REFERENCES:>@ K. Hirose, HWDO, Atmospheric Environment, 38 (38),pp. 6601-6608 (2004).
>@ K. Nakamachi, HW DO, Bunseki Kagaku, 64 (8) pp.
594 (2015).
>@ N. Hagura, HW DO., Bunseki Kagaku, 66 (3), pp.
204 (2017).
>@ N. Hagura, et al., Transactions of the Atomic Energy
Society of Japan, 17 (3-4), pp. 111-117 (2018).

&2 1HXWURQDFWLYDWLRQDQDO\VLVIRUVHGLPHQWVSK\WRSODQNWRQODNHZDWHURI/DNH$NDJL2QXPD
Y. Okada , T. Uchiyama , N. Kumagai , N. Hagura ,
H. 0DWVXXUD and Y Iinuma $WRPLF(QHUJ\5HVHDUFK/DERUDWRU\7RN\R&LW\8QLYHUVLW\&RRSHUDWLYHPDMRULQ1XFOHDU(QHUJ\7RN\R&LW\8QL
YHUVLW\

'HSDUWPHQWRI1XFOHDU6DIHW\(QJLQHHULQJ7RN\R&LW\
8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Contamination of radioactive Cs
of Lake Akagi Onuma in Gunma Prefecture was observed
due to the accident at Fukushima Daiichi Nuclear Power
Station. Recently, the levels of radioactive Cs in wakasagi that live there have been slowly decreasing with thedecrease of that of the lake water. In order to clarify thecause of the gradual collapse, we have been investigating
the inhabiting organisms and their surrounding areas for 8
years 1, 2).
This study will be conducted as part of investigating thecontribution of sediments to lake water. In this research,
we investigated lake sediments, phytoplankton, and traceelements in lake water.
(;3(5,0(176 The sediment sample was processed
as in the 2018 report. 22 sediment samples from 10 to
570 mm deep collected in 2015, dried phytoplankton, andfreeze-dried lake water collected at depths 0, 8 and 15 m
in 2018 (wet weight approx. 500 g) was used for the
analysis. These samples were double-packed in a cleanpolyethylene bag. 31 samples (about 50 mg) and comparative standards (JLK1-1, NIES8) were irradiated with athermal neutron flux of 4.68 × 10 <sup> 12 </ sup> n cm
<sup> -for a short time (30 seconds). Neutron flux 5.5 ×
10 <sup> 12 </ sup> n cm <sup> -2 </ sup at 2 </ sup> s<sup> -1 </ sup>, long time (3600 s)> KUR s <sup> -1</ sup>. To monitor neutron flux, approximately 9 mg ofaluminum wire containing 1.5% Sb and approximately 11
mg of Fe wire were doubly packed in a clean polyethylene bag and the sample and comparative standard were
irradiated together.
The irradiated samples were measured by conventional[&gamma;]-ray spectrometry using a coaxial Ge detector.
Analysis of [&gamma;]-ray spectrometry were at Gamma
Studio (SEIKO EG&G Co.,LTD).
5(68/76 Using neutron activation analysis, 30 elements in sediment, 19 elements in phytoplankton, and 17
elements in lake water were quantified. Fig. 1 shows thestable Cs concentration in each sediment. The stable Csconcentration changes in the range of 2 μg / g to 5 μg / g
at a depth of 10 mm to 570 mm. Among the 19 elementsof phytoplankton, it was found that Mg, Mn, Si, Sb and Cs
have similar concentrations to those of sediments. Fig. 2
shows a comparison of sediment and phytoplankton
smples with Mg, Mn, Si, Rb, Sb and Cs concentrations.

Fig. 3 shows stable cesium quantification results collected in lake water in August 2018. Stable Cs quantification values for unfiltered and filtered lake water are
shown at depths of 15 m, 8 m, and 0 m, respectively.
The stable cesium concentration was highest at 15 m.
This was the same trend as the radioactive cesium concentration in August. Comparing stable cesium with andwithout filtration, both 15 m and 8 m showed similarvalues. From this result, it is considered that stable cesium exists in a dissolved state. At 0m, stable cesium wasfound to be low with filtration and in suspension collected by 0.45μm filter.
5()(5(1&(6[1]K.Suzuki HW DO, Science of the Total Environment,(2018)1153-1164.
[2] M.Mori HW DO, Science of the Total Environment,(2017)1247-125

31053

‑182‑

&2

)RUPDWLRQDJHRI3UHFDPEULDQPHWDPRUSKLFURFNVDQGWKHUPDOKLVWRU\

H. Hyodo1, K. Sato1,2,3, H. Kumagai3and K. Takamiya4,QVWLWXWHRI)URQWLHU6FLHQFHDQG7HFKQRORJ\
2ND\DPD8QLYHUVLW\RI6FLHQFH
'HSDUWPHQWRI$SSOLHG&KHPLVWU\DQG%LRFKHPLVWU\1DWLRQDO,QVWLWXWHRI7HFKQRORJ\)XNXVKLPD&ROOHJH
3
6XEPDULQH5HVRXUFHV5HVHDUFK&HQWHU-DSDQ$JHQF\
IRU0DULQH(DUWK6FLHQFHDQG7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21Acasta gneiss is known as a part ofthe oldest crust (ca. 4.0 Ga) by U-Pb zircon SHRIMP
dating [1]. The thermal history of the rock seems to becomplicated [2] because it shows much younger age (1.9Ga) in apatite U-Pb method [3].
K-Ar system is more susceptive to external disturbancecompared to U-Pb system, and wide range of closure
temperature. To elucidate the thermal history, hornblendeand biotite samples of Acasta gneiss were dated by40
Ar/39Ar method.
(;3(5,0(176 Experimental procedure is the sameas described as previous studies on single grain datings.
Rock samples were crushed and sieved in #25-100 mesh.
After ultrasonic cleaning in distilled water, single mineral
grains were handpicked. The mineral grains were irradiated in the KUR for 24 hours at 1 MW. The total neutron
flux was monitored by 3gr hornblende age standard [4],[5], which was irradiated in the same sample holder. In
the same batch, CaSi2 and KAlSi3O8 salts were used forinterfering isotope correction. A typical J-value was(5.390 + 0.068) X10-3. In stepwise heating experiment,
the minerals were heated under defocused argon ion laser
beam, and temperature of sub-millimeter grains wasmeasured using infrared thermometer whose spatial resolution is 0.3 mm in diameter with a precision of 5 degrees. In order to achieve a precise temperature control,
feedback system between temperature monitoring andlaser power control were adopted. Extracted argon isotopes were measured using the custom made mass spectrometer with mass resolution of approximately 400 to
separate 39Ar peak from neighboring hydrocarbon peak[5].5(68/76 One of 40Ar/39Ar age spectra of biotite grains
were illustrated in Fig. 1. The plateau age 1.935 Ga is
consistent with 1.964 Ga of the hornblende and the U/Pb
age of apatite of the Acasta gneiss, considering a prolonged thermal history.
The area known to have a metamorphic history caused by

Fig. 1. 40Ar/39Ar age spectra of a biotite grain fromAcasta gneiss. The 37Ar/39Ar error seems to be large,
but little effect on the age spectra with a well-definedplateau.
Wopmay orogen around 2.0 Ga. On the other hand, zircons from the area typically show 4.0 Ga. The age gap
seem to represents the difference in closure temperatureof minerals.
Closure temperature depends on the grain size and cooling rate of the orogen. If we apply typical closure temperatures of hornblende and zircon, The Acasta area washeated to at least above 500oC and below 900oC, and thezircon preserved the formation age, but the hornblende
was reset by the Wopmay metamorphism.
5()(5(1&(6>@ S.A.Bowring and I.S. Williams, &RQWULEXWLRQV WR
0LQHUDORJ\DQG3HWURORJ\, (1999) 3–16.
>@ T. Iizuka HW DO 3UHFDPEULDQ 5HVHDUFK  (2007)208.
>@ Y. Sano, HW DO *HRFKLPLFD &RVPRFKLPLFD $FWD (1999) 899–905.
>@ J.C. Roddick, *HRFKLP&RVPRFKLP$FWD  (1983)
898.
>@ H. Hyodo, *RQGZDQD5HVHDUFK  (2008) 609-616.



‑183‑

&2

A Study on Evaluation of Redox Condition of Tokyo Bay using Redox Sensitive
Elements as an Indicator by Means of Instrumental Neutron Activation Analysis

M. Matsuo1, K. Shozugawa1, Y. Guan1, M. Komori1, 2, R.
Okumura3, Y. Iinuma3 and K. Takamiya3
1

Graduate School of Arts and Sciences, The University ofTokyo
2
Yokohama Environmental Science Research Institute3
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: Hypoxia is water mass that is deficient in dissolved oxygen (DO), often occurs in closed
water areas such as the inner bay [1]. In dredged trenchesof Tokyo Bay severe hypoxia has been observed in annual summer seasons. The purpose of this study is to clarify
the relationship between hypoxia and the sediment environment of dredged trench by chemical analysis of sediments in the vertical direction, assuming that the effect ofpast hypoxia could be preserved as a difference in concentrations and/or chemical states of elements in thesediments.
To estimate the sedimentary environment related toredox conditions, various elements have been used. For
example, Fe and Mn are used because their various
chemical states on Eh-pH diagrams have become clear[2]. And U is used for the evaluation of weak reductive
conditions because the redox potential of U(VI)/U(IV) is
between Mn(IV)/Mn(II) and S(VI)/S(-II) [3]. In thisstudy, concentrations of Fe, Mn, U, Th, and Ce in thesediments were analyzed by instrumental neutron activation analysis (INAA).
EXPERIMENTS: We sampled sediment cores fromthe dredged trench and non-dredged seabed off Makuhari,
Chiba Prefecture in August 2019. All cores were cut inthe vertical direction at 2 cm intervals in the laboratory.
Then, the samples were desalted by centrifugation withpure water washing three times and dried at 105 Υ.
Approximately 30 mg of sediments were packed indouble polyethylene film bags to perform INAA. All
samples were irradiated with neutrons at the pneumatictube, Kyoto University Research Reactor. Three types ofgamma-ray measurement were carried out corresponding
to half-lives of elements. For analysis of Mn, samples
were irradiated for 10 seconds at 1 MW, and then gamma-ray was measured for 600 seconds by Ge detector
after 600 seconds cooling. Regarding U, samples were
irradiated for 20 minutes at 1 MW, and then gamma-ray
was measured for 1400 seconds after 3-4 days cooling.
Regarding Fe, Th and Ce, samples were irradiated for 20
minutes at 1 MW, and the measuring time of gamma-ray
was for 10000 seconds after 2-3 weeks cooling.
RESULTS: The concentration of Mn was lower indredged trench than that in non-dredged seabed, suggesting that the dredged trench was in more reductive condition (Fig. 1). On the other hand, there was no significant
difference for Fe. It is well-known that the concentrations

Fig. 1. Depth profile of Mn concentration in thesediments collected from dredged trench (MD) andnon-dredged seabed (MR) off Makuhari.

Fig. 2. Th/U-Ce/U plots in the sediments collectedfrom dredged trench (MD) and non-dredged seabed(MR) off Makuhari.
of both Fe and Mn in sediments increase when conditionof seawater is oxidative. However, we note that Mn precipitates under more oxidative conditions. Therefore, it isestimated that the oxidation-reduction potential in thedredged trench remained to the extent that Fe precipitation occurred but no Mn precipitation occurred.
In addition, we plotted the relation between Th/U andCe/U ratios (Fig. 2). The values of Th/U and Ce/U ratios
at each site existed on a same line. This fact indicates thatthe sediments cannot be the mixture of two or more
sources which have different Th/U and Ce/U ratios.
However, this figure shows that MD samples are in moreoxidative condition. Also, comparing the MD sample
ratios with the values of 2017-year sample shows that thedredged trench in this year is more oxidative. This factindicates that the anoxic state is gradually recovering.
REFERENCES:[1] R.J. Diaz et al., Science, 321 (2008), 926-929.
[2] D.G. Brookins, in Eh-pH diagrams for geochemistry(Springer-Verlag, 1988).
[3] D.R. Turner, M. Whitfield and A.G. Dickson, Geochim. Cosmochim. Acta, 45 (1981), 855-881.

31061

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&2$EVRUSWLRQRIDONDOLPHWDOLRQVE\ZKLWHUDGLVKVSURXWV

M. Yanaga, K. Ogawa1, T. Nagakura1, H. Yoshinaga2,
R. Okumura2 and Y. Iinuma2&HQWHUIRU5DGLRVFLHQFH(GXFDWLRQDQG5HVHDUFK)DFXOW\RI6FLHQFH6KL]XRND8QLYHUVLW\
1'HSDUWPHQW RI &KHPLVWU\ )DFXOW\ RI 6FLHQFH 6KL]XRND
8QLYHUVLW\2,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The Fukushima Daiichi Power
Plant accident caused a large amount of radioactive materials released in to the atmosphere[1-3]. Radioactive cesium is especially a problem because of its long half-life.
Paddy field soil was also contaminated with radioactive
cesium. However, simple removal of contaminated soil
would create a vast quantity of radioactive waste. Therefore, separating radioactive cesium from the soil is necessary to prevent damage by rumors and to minimize thequantity of radioactive waste.
Previously, we reported that the absorption of radioactive cesium from artificially contaminated soil into
rice plants increased by adding a stable isotope to irrigation water and that the possibility that the cesium atoms
added were replaced with radioactive cesium atoms insoil [4, 5]. However, addition of excess amount of stable
cesium caused an obstacle to growth of rice plant [6].
Therefore, in this study, we conducted hydroponic cultureof white radish sprouts and analyzed trace elements contained in leaves and stems to investigate the behavior ofcesium added to the culture solution and the competitive
relationship between alkali metals.

cesium ions to the culture solution. When only cesium
ions were added to the culture medium, the cesium concentration in the leaves increased with the growth of thewhite radish sprouts, indicating that cesium ions wereabsorbed and accumulated in the leaves. Furthermore, as
shown in Fig. 1, when grown in a mixed solution withrubidium ions, the cesium concentration in leaves increased. Increasing the concentration of rubidium ions in
culture medium increased the cesium concentration in theleaves. This suggests that rubidium ions promoted absorption of cesium ions by plants. However, when thecesium ion concentration in the culture solution was tripled, the leaves discolored and growth disorders wereobserved. On the other hand, when cesium and potassiumions were added in culture medium, cesium concentrationin leaves decreased as the potassium ion concentration in
medium increased. This suggests that the presence ofpotassium ions suppress absorption of cesium ions inplants.

(;3(5,0(176 0DWHULDOV DQG 0HWKRG
Cultivationof white radish sprouts was carried out by adding alkali
metal ions, such as potassium ions, rubidium ions and/or
cesium ions, to a diluted solution of a commercially obtained culture solution, HYPONeX (HYPONeX JAPAN CORP.,LTD.).
,1$$ The samples in polyethylene capsules were irra-diated in Pn-3 for 90 seconds and in Pn-2 for 4 hours,
for short and long irradiation, respectively. As comparative standards, the certified NIST Standard Reference
Mate-rial 1577b Bovine Liver as well as elemental
standard for Cs was used. The J-ray spectroscopic
measurements with an HPGe detector were performed
repeatedly for the short-irradiated samples: the firstmeasurements for 120 ² 900 seconds after decay time of
5 - 15 minutes and the second one for 250 - 1200 seconds
after 60 - 150 minutes. The long-irradiated samples
were measured for 1 - 24 hours after an adequate coolingtime (15 - 60 days).
5(68/76 In order to examine the change in the concentration of cesium ions contained in the leaves, whiteradish sprouts were cultivated by adding 3.0 u 10-5 mol ofFig. 1. Cesium ion concentration in leaves of whiteradish sprouts grown in culture solutions with various alkali metal in concentrations. The amount of
cesium ion added to the culture solution was constant
and was 3.0 u 10-5 mol.

5()(5(1&(6>@ S. Endo et al., J. Environ. Radioact., 111(2012)18-27.
>@ 0Yanaga and Y. Oya, Radiation Safety Manage-ment,12(2013)16-21.
>@ 0Yanaga et al., Radiation Safety Management, 12(2013)37-42.
>@ M. Yanaga HWDO, NMCC ANNUAL REPORT, 22(2015)185-190.
>@ M. Yanaga HWDO, NMCC ANNUAL REPORT, 23(2016)172-179.
>@ M. Yanaga HWDO, KURNS Progress Report 2018(2019)CO5-10.

31064

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&2INAA and Ar-Ar Dating for Micro-sized Extraterrestrail Materials

R. Okazaki and S. Sekimoto'HSDUWPHQWRI(DUWKDQG3ODQHWDU\6FLHQFHV.\XVKX8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: The major goal of this study is todetermine the minor element compositions and Ar-Ar
ages for submillimeter-sized extraterrestrial materials. We
have been continually working to achieve this objective
since 2013 (project #: 25066, PI: S.S.). In the Ar-Ar dating, concentrations of the parent (40K) and daughter(40Ar) nuclides are determined simultaneously. In order toobtain precise ages, it is important to adjust the irradiation condition, such as irradiation duration, neutron fluxand neutron energy.
In the last year’s proposal, we have investigated two irradiation conditions by using the hydraulic conveyor andthe long-term irradiation plug. We have measured noble
gases in JG-1 and orthoclase samples irradiated by the
Hydro and Long-term irradiations. Based on the 39Ar/40Ar
ratio determined for the Hydro and Long-term orthoclase
samples, we found that the neutron flux parameter(J-value) for the Long-term irradiation is about half ofthat for the Hydro irradiation. Especially for NAA, it isimportant to evaluate the difference in the neutron energy
spectrum between the two irradiation conditions. In thisyear’s proposal, we conducted NAA for the standard
minerals and a meteorite sample (Allende) that was already measured for NAA previously by using the Hydro
irradiation.

minor element concentrations in DTS-2b and JP-1 will
also be calculated and compared with the compositions
reported [3, 4].
After the gamma ray measurements, some of the irradiated samples were moved to Kyushu Univ. to measurenoble gas isotopes. Noble gas analyses for these samples
will be done this summer in order to evaluate the presence of interference isotopes produced by the low energy
neutrons.
REFERENCES:>@ E. Jarosewich et al., Smithsonian Contributions to the
Earth Sciences 27 (1987) 1-49.
>@ A. Ando et al., Geochemical Journal 5 (1971)
151-164.
>@ https://gbank.gsj.jp/geostandards/igneous.html>@ I. Raczek et al., Geostandards Newsletter, 25 (2001)
77-86.
>@ S. Weiss, Mineralien Magasin Lapis. 16 (1991)
13–14.

EXPERIMENTS: Several hundred milligram samples
were prepared from the Allende CV chondrite (Provided
by Smithonian museum [1]) and our standard minerals(JB-1 [2], JP-1 [3], DTS-2b [4], orthoclase [5], sanidine,
and wollastonite). Each of the samples was placed in a
conical dimple (φ1, depth ~ 0.5 mm) of a sapphire disk
(φ5.5, 1.5 mm thick), and covered with a sapphire disk
(φ5.5, 0.3 mm thick). Each of the sapphire container was
wrapped with pure aluminum foil. These Al-wrapped
containers were stacked and sealed in the capsules for theLong-term irradiation. Condition of the Long-term irradiation as 122 hours under 1MW-operation + 18 h under
5MW-operation.
REUSLTS and DISCUSSION: After irradiation, thesamples were moved to non-irradiated glass container
with similar dimension from the sapphire one in order toreduce the radioactivity from the sapphire containers andAl foil. For the selected samples (Allende, JP-1, andDTS-2b), gamma ray measurements of radioactive nuclides were performed. The results are now analyzed to
examine if the gamma ray spectrum of the Long-term
irradiated Allende sample is essentially identical to theprevious result of the Hydro irradiation. Based on the
spectrum of the Long-term irradiated Allende sample,

31068

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‑188‑

togi vain (n=14)
Central value = 8.2 ± 1.4 (1σ)

23Dispersion = 57 %P(χ²) = 0.00

15
2
0
-2
10

Peak 1: 3.11±0.18 (15.1±9.9%)5

Peak 2: 6.02±0.48 (25±15%)2

Peak 3: 13.013±0.06 (60±18%)
σ 20

0.1

0.06

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'HSDUWPHQWRI(DUWK6FLHQFHV:DVHGD8QLYHUVLW\,1752'8&7,21  Howardite, eucrite and diogenite(HED meteorites) are the largest group of achondrite
which are thought to have been derived from asteroid
Vesta. Recently, the Dawn mission confirmed that the
Vesta’s surface is mineralogically and chemically similar
to HED meteorites [1]. Depletions of siderophile elements in HED meteorites suggest that HED meteorites areproducts of differentiation [2]. Therefore, HED meteorites are important to elucidate the core formation of Vesta.
Eucrites are mostly composed of pyroxene and plagioclase. As almost all eucrites are brecciated, it is difficult
to bring out their primitive chemical compositions. Someeucrites (e.g., ALH 76005) were reported to contain foreign meteoritic components [e.g., 3]. From these materials, siderophile elements abundances for eucrites may
have been modified. A few unbrecciated eucrites also
have been found. As siderophile elements abundances forthese unbrecciated eucrites were not affected by the incorporation of foreign materials, its chemical compositions give us the important information about the differentiation processes of Vesta. We determined elemental
abundances for Northwest Africa (NWA) 10962, which
was classified into unbrecciated eucrites [4] by using
INAA and aimed to chemically characterize this meteorite in comparison with those for other eucrites.
(;3(5,0(176 A chip of NWA 10962 weighing 1.4
g was carefully ground in an agate mortars in order toobtain the representative chemical composition. This
powder sample was firstly irradiated for 10 s at the pn-3of the Institute for Integrated Radiation and Nuclear Science, Kyoto University with thermal and fast neutron
fluxes of 4.6 x 1012 and 9.6 x 1011 cm-2s-1, respectively.
After irradiation, sample was immediately measured for
gamma-ray emissions. After 24 hours, the same sample
was irradiated fro 3 h at the pn-2 of the Institute for Integrated Radiation and Nuclear Science, Kyoto University,with thermal and fast neutron fluxes of 5.6 x 1012 and 1.2
x 1012 cm-2s-1, respectively. The sample was measured
three times for gamma-rays after different cooling intervals over a one-month period. JB-1 and the Smithsonian
Institution Allende meteorite sample were used as thestandard reference material.
5(68/76 $1' ',6&866,216 Twenty elements
could be determined by using INAA. Major elementsabundances of NWA 10962 are similar to those of thecommon Main-group eucrites. However, it is noticed that
trace element abundances of NWA 10962 are slightly
different from those of the common Main-group eucrites.
La abundances are plotted against Hf abundances for

eucrites in Fig. 1. On this plot, eucrites are classified into
the three subgroups; cumulate eucrites, basaltic eucrites
and residual eucrites [5]. As clearly confirmed in Fig. 1,
NWA 10962 belongs to residual eucrites. In terms of rareearth elements (REEs) abundances, NWA 10962 is different from the common eucrites. NWA 10962 is slightly
depleted in light REEs. Its REE pattern exhibits a pronounced positive Eu anomaly, which bears some resemblance to cumulate eucrites and residual eucrites. Thus,
NWA 10962 is classified as residual eucrites.

Fig 1. La vs. Hf for euceites.

Based on petrology [4], it was reported that NWA 10962
contain about 1% of FeNi metal. It is examined whether
this FeNi metal endogenously produced or not based on
its elemental abundances. To extract FeNi metal, the irradiated sample was leached with 6M HCl in an ultrasonicbath for 10 min. The obtained solution was measured by
gamma-ray emissions. For this solution, Fe and Co could
be determined, while Ir and Ni could not be detected.
Nickel/Co and Ir/Co ratios of NWA 10962 are different
from those of iron meteorites and FeNi metal for chondrites. These elemental ratios of NWA 10962 are lower
than those of FeNi metal of Camel Donga, which wasconsidered to be produced by reduction of FeO and FeS[6]. Thus, FeNi metal of NWA 10962 is not foreign meteoritic components and it is concluded that NWA 10962
is suitable for discussing about differentiation of asteroid
Vesta.
5()(5(1&(6[1] M. C. De Sanctis HWDO, Science, (2012) 697-700.
[2] K. Righter and M. J. Drake, Meteorit. Planet. Sci., (1997) 929-944.
[3] N. Shirai HW DO, Earth Planet. Sci. Lett.,  (2016)57-65.
[4] A. Bouvier HW DO, Meteorit. Planet. Sci.,  (2017)2411.
[5] A. Yamaguchi HWDO, Geochim. Cosmochim. Acta, (2009) 7162-7182.
[6] H. Palme HWDO, Meteoritics, , 49-57 (1988).

31081

‑189‑

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6SDWLDO'LVWULEXWLRQRI+DORJHQ&RPSRVLWLRQVLQWKH:HGJH0DQWOH
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H. Sumino, J. Ren, A. Takenouchi, M. Koike, R. Okumura1, Y. IInuma1, H. Yoshinaga1 and S. Sekimoto1
8QLYHUVLW\RI7RN\R ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Mantle wedge - the triangularshaped piece of mantle that lies above subducted plate(slab) and below the overriding plate - is essential fortransporting water into mantle at subduction zone. The
oceanic plate is hydrated before subducting, and thendehydrates at subduction zone to supply water to themantle wedge. However, the details of hydration and dehydration processes remain debated. A major question isthe exact depth where water is released, because water
would notably change the chemical and physical properties of rocks and play an important role in volcanism andseismicity at subduction zones.
The heavy halogens (Cl, Br, I) are highly soluble in fluids,
and hard to enter minerals during partial melting of peridotite (the major type of rock in the mantle) [1]. Furthermore, their ratios, especially I/Cl ratios vary up to
several orders of magnitude among different reservoirs in
subduction zones (e.g. mantle, subducting slab, sediments,and sedimentary pore fluids – water trapped in pore spacein sediments), making them good tracers for fluid sourcesin subduction systems [2,3].
In this study, we analyzed the halogens in rock samples
of an ancient slab-wedge mantle boundary [4] and observed the spatial distribution of halogen compositions, inorder to constrain how the fluids from subducted plate
modified the mantle wedge and how volatiles moved in
subduction zones.
6$03/(6 $1' %$&.*5281' The Sanbagawa
belt, which lies on the south of Median Tectonic Line, iscomposed of various kinds of metamorphic rocks which
experienced subduction to deep in the Earth. It is proposed that Shiraga metaserpentinites (hydrated and deformed peridotites) in the Sanbagawa belt are originatedfrom wedge mantle. Further, a previous study shows thatthe eastern boundary of Shiraga metaserpentinite preserved primary information about the ancient slab-wedge
mantle interface [4]. In contrast, various types of schists
represent altered slab materials that surrounding serpentinite body.

nal fluid that reacted with rocks. While the data obtainedwith heating of residual powder after crushing mainly
represents the composition of halogens in solid phase, i.e.
crystal lattice of minerals. 
5(68/76 The halogen data of crush extraction show
markedly higher I/Cl (1.5 × 10–4 – 3 × 10–3) comparing
with normal upper mantle (4 × 10–5), seawater (~10–6),
oceanic crust (~10–6 – 10–7), or other reservoirs in subduction system. This is similar to the mantle wedge peridotites that come from ~100 km depth [2], which areconsidered to originate from sedimentary pore fluids at
seafloor.
It is notable that “Si-rich serpentinite”, samples near theslab wedge mantle boundary have evidently higher I/Cl
than others. Within the serpentinite body, I/Cl tend to
decrease with the distance from the boundary, whichmeans that the original fluid with high I/Cl may comethrough/from the slab wedge mantle interface, then diffused upward into the mantle wedge and was gradually
diluted by normal mantle with low I/Cl. In addition, thistrend is not continuous at the slab wedge mantle boundary, implying the original fluid not necessarily came directly from the adjacent slab materials.
&21&/86,216: The halogens composition of Shiraga serpentinite body shows similar elemental ratioswith that from deeper mantle wedge peridotites, which
are considered to originate from the same source as sedimentary pore fluids. Based on the spatial distribution of
I/Cl, the original fluid could come through slab wedge
mantle interface, and then transfer upward into the mantle
wedge.
5()(5(1&(6[1] D. M. Pyle & T. A. Mather. Chem. Geol.,  (2009)110-121.
[2] H. Sumino HWDO, Earth Planet. Sci. Lett., (2010)
163-172.
[3] M. A. Kendrick HW DO, Earth Planet. Sci. Lett., (2013) 86-96.
[4] H. Kawahara HWDO, Lithos,  (2016) 53-66.
[5] N. Ebisawa HW DO, J. Mass Spectrom. Soc. Jpn., (2004) 219-229.

(;3(5,0(176 Samples were neutron irradiated in
KUR to convert halogens (37Cl, 79Br, 127I) to noble gas
proxies (38Ar, 80Kr, 128Xe). The extraction (crushing andheating) and measurement of these noble gas proxies
were analyzed with a mass spectrometer at the Universityof Tokyo [5]. The crushing method releases halogen-derive noble gases from fluid inclusions, which arethought to partially preserve the information of the origi-

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Fission track age and thermal history of clay deposit of the Tsuchihashi Mine

H. Ohira and Y. Sampei
Department of Earth Science, Shimane University
INTRODUCTION: Fission track (FT) dating was carried out to estimate ages of hydrothermal alteration toform clay deposit of the Mitsuishi mining area at Bizen
City, Okayama prefecture. Several clay deposits are located near the ring fault of eastern margin of the Wake
Caldera, implying that hydrothermal fluid circulation
along the ring fault contributed to form the deposit of thisarea [1]. The Tsuchihashi mine is typical mine operating
underground quarry, yields high grade clayey rocks used
for raw materials of refractories and ceramics. Several
zones (such as pyrophyllite, sericite and silica rock) develop in response to conditions of hydrothermal alteration [2]. Samples were collected from above zones andU-Pb dating was also applied to estimate eruption age ofhost pyroclastic rocks.
EXPERIMENTS: Sample was crashed, sieved andheavy minerals were concentrated using conventional
method of heavy liquid and magnetic separator. Minerals
were mounted in PFA Teflon, and polished to reveal acomplete internal surface, and etched in NaOH-KOH
eutectic melt at 225˚C [3] for 12-15 hours. Samples were
irradiated at pneumatic tube of graphite facility (Tc-pn)of Kyoto University Reactor (KUR). After irradiation,
external detectors (mica) were etched in 46% HF at 25˚C
for 6-7 minutes (for mineral mounts) and for 20-50min(for NIST-SRM612 glass). FT density was measured at
1000× magnification with a dry objective. U-Pb dating
was carried out in cooperation with Dr. Hisatoshi ITO ofCentral Research Institute of Electric Power Industry(CRIEPI). Dating was performed using a Thermo Fisher
Scientific ELEMENT XR magnetic sector-field ICP-MS
coupled to a New Wave Research UP-213 Nd-YAG laser
at CRIEPI [4].
RESULTS: FT ages obtained are 72.4±2.5Ma and72.6±2.6Ma (silica rock zone), 75.9±2.7Ma (pyrophyllitezone) and 77.9±3.4Ma (sericite zone). These FT ages are
relatively compatible with previously reported K-Ar ages
for clay veins (78.1Ma, 74.0Ma, 73.0Ma) and clayey
rocks (80.0Ma, 78.8Ma, 77.8Ma) [5]. Newly obtained
U-Pb ages are 78.0 s 1.5Ma (silica rock zone 㸧 and
77.3±1.8Ma (sericite zone). These ages are slightly
younger than previously reported age (82.4±0.6M [2]).

Ages versus closure temperature plot are shown in Fig. 1.
U-Pb ages probably correspond to stage of eruption ofhost pyroclastic rocks or magmatic activity causing caldera structure, considering with its high closure temperature (800 Υ < [6]). The variation of U-Pb ages
(77-82Ma) should be examined in more detail. Previously reported K-Ar age (73-80Ma, [5]) probably correspond to a period of culmination of hydrothermal activity
which formed several clay zones after caldera formation.
Considering relatively lower closure temperature of FT
methods (230Υ<), FT ages (73-78Ma) probably indicate
a period when sample cooled below 240Υ during attenuation of hydrothermal alteration. The youngest FT
age from silica rock zone (72.4-72.6Ma) show a periodof latest stage of hydrothermal activity, which was probably sustained for a certain period (several Ma) after
eruption of host pyroclastic rocks or caldera formation.
Period of eruption of
pyroclastic rock andcaldera formation

Period ofhydrothermal
alteration

Silica rock zone
(final stage offhydrothermal
activity)

Pyrophillite andSericite zone

Fig.1 Closure temperature vs. Age plot.
>@ ISHIHARA S. and IMAOKA T., 1999, Resource Geology, 49, 157-162.
>@ Sato D., Yamamoto T. and Takagi T., 2016, Geologyof the Banshu-Ako district. Quadrangle Series,
1:50000, Geological Survey of Japan, AIST, 68p (inJapanese with English abstract).
>@ Gleadow A.J.W. et al., 1976, Earth and Planetary
Science Letter, 33, 273-276.
>@ Ito H. HW DO 2017, Quaternary Geochronology 40,
22.
>@ Hongu H., Kitagawa R. and Nishido H., 2000, Clay
Science (Nendo Kagaku) 40, 46-53.
>@ Cherniak, D.J. and Watson, E.B., 2000, Chemical.
Geology, 172, 5

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40Ar-39Ar Dating of Extraterrestrial Materials in KURNS

N. Iwata, S. Sekimoto1, R. Okazaki2 and Y. N. Miura3
Faculty of Science, Yamagata University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Department of Earth and Planetary Sciences, Kyushu
University
3
Earthquake Research Institute, University of TokyoINTRODUCTION: Radiometric dating is useful toolfor unveiling formation and evolution process of planetary material. 40Ar-39Ar method is invaluable to date thetiming of heating events on planetesimal and asteroid (e.g.
Swindle et al. (2014) [1]). Especially, 40Ar-39Ar dating
method with laser heating technique is suitable for small
amount sample (e.g. Kelley, 1995 [2] and Hyodo, 2008[3]).
For example, tiny material returned from asteroid
25143 Itokawa is dated using laser heating 40Ar-39Ar dating method by Park et al. (2015) [4] and Jourdan et al.
(2017) [5]. Park et al. (2015) reported an age of 1.3 ± 0.3
Ga. Jourdan et al. (2017) reported an age of 2.3 ± 0.1 Ga.
These ages indicate the timing of catastrophic events
which were occurred on Itokawa’s precursor body. Combining the 40Ar-39Ar ages and other chronological data,
Terada et al. (2018) [6] overviewed the time evolution of
the Itokawa asteroid. Similar investigation, the integration of multichronological data is proposed to the material that recovered from asteroid 162173 Ryugu and otherextraterrestrial materials. 40Ar-39Ar dating will play animportant role within the investigations.
To implement of dating of extraterrestrial material
by 40Ar-39Ar method, we will develop a system which
includes gas extraction and gas purification line in
KURNS (Fig. 1). A continuous Nd-YAG laser (~60 W)
extract gas from neutron irradiated sample. The extracted
gas is purified and encapsulated into metal gas trap. The
purified gas in the metal gas trap is transported to laboratories of noble gas analysis (e.g. Kyushu University) andargon isotope of the gas is analyzed using noble gas mass
spectrometer. Further, we have a plan to connect a quadrupole mass spectrometer to this system in the future, inorder to perform on-lined laser heating 40Ar-39Ar dating.
EXPERIMENTS: Dr. R. Okazaki of Kyushu University designed the system. The gas extraction part consistsof a sample chamber. The gas purification part consists ofa Sorb-AC getter pump. Ti-Zr getter will be added asneeded. Connecting port is used for jointing gas purification part and gas trap tree and/or the quadrupole mass
spectrometer as needed. Whole of the parts are evacuatedby two oil rotary pumps and two turbo molecular pumps
to ultra-high vacuum condition.

Fig. 1. Outline of gas extraction and purification line in
KURNS. Components in parentheses are optional.
RESULTS: We started assembling of the laser-heating
gas extraction and purification system in KURNS in 2019.
The design work and configuration of the system is almost completed. Unfortunately, the constructing work
was interrupted by influence of epidemic prevention of
COVID-19. We are going to continue setting the system
up during 2020.
REFERENCES:[1] T. D. Swindle et al., in Advances in 40Ar/39Ar Dating:from Archaeology to Planetary Sciences, edited by
Jourdan, Mark, Verati (Geol. Soc., London, Spec. Pub.
378, 2014) 333-347.
[2] S. P. Kelley, in Microprobe techniques in the earthsciences, edited by Potts, Bowles, Reed, Cave
(Chapman & Hall, London, 1995) 327-358.
[3] H. Hyodo., Gondwana Res. 14 (2008) 609-616.
[4] J. Park et al., Meteorit. and Planet. Sci., 50 (2015)
2087-2098.
[5] F. Jourdan et al., Geology, 45 (2017) 819-822.
[6] K. Terada et al., Sci. Rep., 8 (2018) #11806.

31126

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1HXWURQ DFWLYDWLRQ DQDO\VLV RI FDUERQDWH UHIHUHQFH PDWHULDOVFRUDO -&S  DQG JLDQW FODP -&W 

S. Sekimoto, Y. Homuraa, V.D. Ho1, M. Inagaki, N. Shirai2, T. Ohtsuki,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
1XFOHDU5HVHDUFK,QVWLWXWH9LHWQDP$WRPLF(QHUJ\,Q
VWLWXWH
'HSDUWPHQWRI&KHPLVWU\7RN\R0HWURSROLWDQ8QLYHUVLW\D
3UHVHQWDGGUHVV1RYDOWLV)DUPD,1752'8&7,21  Geochemists are often interested
in the abundance of halogen elements in geochemicalmaterials such as crustal rocks, mantle materials, andmeteorite samples, because halogens play an importantrole in investigating the petrogenesis of such materials
and assist in tracing their origins and/or precursor materials [1-3]. In our previous work, radiochemical neutron
activation analysis (RNAA) was refined to accurately
determine even trace amounts of halogens (chlorine,
bromine, and iodine) in sedimentary rock reference samples [4]. Subsequently, U.S. Geological Survey (USGS)
geochemical reference materials were subjected to
RNAA, and the data obtained were compared with literature data [5]. The two kinds of carbonate reference materials investigated here, JCp-1 (Coral) and JCt-1(Giant
Clam), are prepared by the Geological Survey of Japan/National Institute of Advanced Industrial Science andTechnology (GSJ/AIST), and the concentrations of many
major and a few trace elements in these materials havebeen determined [6-8]. Data about the halogen contents
in these materials is expected to significantly contributeto a better understanding of the chemistry of seawater andthe marine environment, since halogens (especially iodine) are known to be extremely useful in investigating
the geochemical circulation of terrestrial materials [9].
However, to our knowledge, there is not much data on the
halogen contents of these carbonate materials.
The present study aims to use RNAA and instrumental
NAA (INAA) to determine trace amounts of three halogens in JCp-1 and JCt-1, together with other elements.
Based on the halogen data, the differences between thetwo carbonate reference materials is investigated. The
INAA values obtained in the present study are comparedwith literature values, and the consistency between ourdata and the data from known literature is evaluated.
(;3(5,0(176 The procedure of RNAA used inthis work has been reported previously.[4] For INAA
studies, about 50 mg of JCp-1 and JCt-1, together with asimilar amount of two kinds of USGS basalt referencematerials for quantification, BCR-2 and BHVO-2, wasirradiated for 4 h using KUR to measure the relatively
long-lived nuclides (with half-lives > 24 h; 46Sc, 59Fe,
60
Co, 85Sr, 134Cs, 140La, 141Ce, 152Eu, 181Hf, and 182Ta, and239Np) produced by the (n,J) reaction in each material. As
for 239Np, the (n,J) reaction is followed by J-decay. Addi-

tionally, the nuclides 24Na, 28Al, and 49Ca in these materials were also measured by irradiating the samples for 10 s.
Since the Mn content in the two carbonate materials ofinterest in this study (JCp-1 and JCt-1) is known to bevery low relative to that in geochemical materials, irradiation for 20 min was required for the measurement of56
Mn. For determination of the Mn content, a chemical
standard solution of Mn was utilized. An appropriate
amount of Mn solution (100 mg kg-1, typically) was
dropped onto a filter paper, which was then dried under
an infrared lamp. The filter paper was then doubly sealedin polyethylene bags, and after irradiation, the outer bags
were exchanged for new (non-irradiated) ones.
5(68/76 The contents of Cl, Br, and I in JCp-1 andJCt-1 were determined by RNAA and is shown in Table 1.
Uncertainties refer to counting statistics (1V) from gamma-ray spectrometry just after the radiochemical purification, as well as from those in the reactivation process.
Information values for Cl have been reported as determined by spectrophotometry (584 and 95 mg kg-1 in
JCp-1 and JCt-1, respectively) [8], which are in good
agreement with the RNAA values from the present study,
with uncertainties of 3V. The estimates for the Br and I
contents for these two carbonate materials are reported
here for the first time. There is a scarcity of reliable andaccurate halogen data for these materials. It is envisionedthat the halogen data reported using RNAA will contribute to a compilation of such data for a database of
GSJ/AIST reference materials.
7DEOHCl, Br, and I contents in JCp-1 & JCt-1, as estimated by RNAA
Sample Cl(mg kg-1)
Br(mg kg-1)
I (mg kg-1)
JCp-1
620 ± 27
3.22 ± 0.10
6.14 ± 0.15
JCt-1
103 ± 80.301 ± 0.011
0.031 ± 0.005
5()(5(1&(6[1] MA Kndrick HWDO, Geochim. Cosmochim. Acta (2018) 285-304.
[2] L. Hughes HW DO, Geochim. Cosmochim. Acta (2018) 1-23.
[3] DE Harlov HWDO, The Role of Halogens in Terrestrial
and Extraterrestrial Geochemical Processes Springer
Geochemistry, Gewerbestrasse, Switzerland (2018)[4] S. Sekimoto HWDO, Anal. Chem.  (2013) 6336-6341.
[5] S. Sekimoto HWDO., Geostand. Geoanal. Res.  (2017)
213-219.
[6] S. Aizawa, J. Radioanal. Nucl. Chem.  (2008)
349-352.
[7] M. Inoue HW DO., Geostand. Geoanal. Res.  (2004)
411-416.
[8] T. OkaiHWDO., Chikyuukagaku  (2004) 281-286.
[9] B. Deruelle et al., Earth Planet. Sci. Lett.  (1992)
217−227.

31132

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&2Long term analysis of Cs isotopic ratio by thermal ionization mass spectrometry
Y. Shibahara, S. FukutaniDQG T. Kubota,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: The applicability of the mass
spectrometry has been studied for the analysis of radionuclide related to the nuclear incident such as the Fukushima Dai-ichi Nuclear Power plant accident. In the recent studies of our group, a thermal ionization mass spectrometer (TIMS) was applied for the analysis of Cs isotopic composition [1], and it was discussed that the analytical results of Cs isotopic composition obtained within
the latest 2 financial years from April 2017 to March
2019 [2]. In this study, we discussed the additive agent
used in the analysis of Cs isotopic composition by TIMS
and the analytical results of Cs obtained within the latest
3 financial years from April 2017 to March 2020.
EXPERIMENTS: From the environmental sample
obtained in Fukushima prefecture, Cs was recovered according to the recovery scheme discussed at the previous
studies [3-5]. The concentration of 137Cs of this sample
corrected on Mar 11, 2011 was about 2.6×10-10 g/g. The
Cs isotopic composition was analyzed by TIMS as theisotopic ratios of 134Cs/137Cs and 135Cs/137Cs.
A thermal ionization mass spectrometer (TRITON-T1,
Thermo Fishier Scientific) was used for the analysis of
Cs isotopic composition. The Cs sample was loaded ontoa rhenium filament of a single filament system with a
TaO activator or a glucose activator same as the previous
study [2]. Because of the loading amount of Cs (ca.
1×10-12 g), the mass spectrometry was conducted with asecondary electron multiplier detector and the peak jump
method [2-5]. For the discussion of the additive agent
used to the ionization of Cs, about 1×10-12 g of the stableCs (namely 133Cs) was loaded onto a rhenium filament.
TaO or glucose (or diluted them) was used as the additive
agent.
RESULTS: Figure 1 shows the mass spectrum of Cs
recovered from the environmental sample (observed at
Oct 2019), and shows the peaks corresponding to 133Cs,
134
Cs, 135Cs and 137Cs. It was observed that the ionizationof Cs was affected by the kind of the additive agent,
while that was not affected the dilution of additive agentswith the dilution rate among 1 to 10.
The analytical result of 135Cs/137Cs ratio obtained
within latest 3 years was shown in Fig. 2. The averaged
value of 0.365±0.003 was obtained, and this value shows
the good agreement with the previous study [2](0.365±0.004). From the time profiles of 135Cs/137Cs and134
Cs/137Cs, the half-lives of 134Cs and 137Cs were evaluated as T1/2(Cs-134) = 2.07±0.03 y and T1/2(Cs-137) = 30.2±2.2
y respectively. These values also show the good agreement with the previous study [2] (2.08±0.02 y for 134Cs
and 30.2±2.2 for 137Cs) and the literature data [6] (2.07 yfor 134Cs and 30.2 y for 137Cs).

Fig. 1 Mass spectra of Cs recovered from environmental
sample obtained at Fukushima prefecture observed at Oct
2019.

Fig 2 Results of Cs isotopic ratio analysis obtained within
latest 3 years corrected on March 11, 2011.

REFERENCES:>@ Y. Shibahara et al. KURRI progress report 2017, 157.
>@ Y. Shibahara et al. KURRI progress report 2018, 103>@ Y. Shibahara et al. J. Nucl. Sci. Technol. 2014, 51,
575-579.
>@ Y. Shibahara et al. Radiological issues for Fukushima's revitalized future. Springer. 2016. 33-46.
>@ Y. Shibahara et al. J. Nucl. Sci. Technol. 2017, 54,
158-166.
>@ R.B. Firestone et al. Table of Isotopes, John Wileyand Sons, New York, 1998.

31160

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&2

Analysis of Cd and As in the rice seed detected from the remains by NAA

T. Inamura, S. Fukutani1 and K. Takamiya1
Archaeological Institute of Kashihara, Nara Prefecture
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: Parameters of the rice yield at the
Yayoi period have been investigated on the basis of nitrogen supply, paddy structure etc. One of the importantparameters to estimate the yield is the submerged condition of the paddy fields. However, the submerged condition has not been clear yet. It was found that the elemental composition of Cd and As of brown rice is goodindex of the submerged condition by elemental analysis
using ICP-MS for modern rice seeds in the previous work[1]. However, the detected rice seeds which is cultural
assets must be analyzed by a nondestructive method. We
have tried to analyze the concentration of Cd and As ofthe detected rice seed by NAA (neutron activation analysis) using pneumatic irradiation system and normal
Ge-detectors, and succeeded to determine the amount of
As. On the other hand, the amount of Cd could not be
estimated. The seeds buried in the ground contain highamounts of mineral elements compared to fresh seeds,
and the mineral components such as iron and sodium
disturb the determination of Cd by large Compton-background in gamma-ray measurements. In order todecrease the Compton continuum in gamma-ray measurement, determination of Cd using a Ge-detector combined with Compton suppression systemin had been triedin the previous work [2]. But the photo peak of Cd isotopes; 107Cd (t1/2 = 6.5 h), 111mCd (t1/2 = 48.5 m) and 115Cd(t1/2 = 53.5 h), was not detected. In the present work, we
irradiated rice samples using hydraulic irradiation system
of KUR to detect the photo peaks of 109Cd which has
longer half-life of 462 d.
EXPERIMENTS: The buried rice seeds (Fig. 1) andchaffs irradiated in the present work were excavated at
the Daifuku remains in Nara. The main elemental components of the samples were analyzed by EDX (Energy
Dispersive X-ray spectrometry) before neutron irradiation.
It was found that high amount of iron which produces

long half-lived isotopes, 59Fe (t1/2 = 44.5 d), is containedin the rice samples. Several grams of the samples double-sealed with polyethylene bag and aluminum foil was
encapsulated in an aluminum capsule. Neutron irradiation
for the samples was performed using the hydraulic neutron irradiation system for 70 hours under 1 MW operation of KUR. After the irradiation, sample stands for threemonths to decrease activities of short-lived nuclides suchas 56Mn, 24Na and also long-lived ones such as 59Fe, 46Sc
(t1/2 = 83.8d) produced by the neutron irradiation. The
gamma-ray spectra of irradiated samples were measured
by a Ge-detector to check the degree of disturbancecaused by long-lived nuclides in the sample.

Fig. 1 The rice seeds sample excavatedat the Daifuku remain.
RESULTS: The activity of 59Fe decrease to about fourthcompared with that at the end of irradiation. However, it
was not low enough to detect photo peaks of 109Cd clearly.
The result suggests longer cooling time is required todecrease the activity of 59Fe and detect photo peaks of109
Cd. In the near future, the gamma-ray measurement
will be carried out under the condition of low activities of59
Fe and other products.
REFERENCES:>@ T. Inamura HW DO., KURRI Progress Report 2017(2018) 208-208.
>@ T. Inamura HW DO., KURRI Progress Report 2018(2019) 189-189.

31165

‑198‑

&2

$QDQ\VLVPHWKRGRIVWURQWLXPLQVHDZDWHU

Y. Ogata, H. Minowa1, S. Kojima2, Y. Kato3 and K. Takamiya4
1DJR\D8QLYHUVLW\
7KH-LNHL8QLYHUVLW\6FKRRORI0HGLFLQH$LFKL0HGLFDO8QLYHUVLW\+LWDFKL/WG,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Conventional analysis methods ofradiostrontium in seawater are complicated and time-consuming using a lot of deleterious substances. We are developing rapid and safe methods[1,2],. In the new method,strontium is collected on a filter with methods using ion
exchange resin or Sr adsorbent, and is measured by a liquid
scintillation counter using plastic scintillator. In this experiment, we tried to analyse behavior of Ba and Na throughthe procedure. First of all, 24Na was measured with modified sum-peak method developed by Ogata[3, 4], also 46Sc
was measured to verify the method. After them, we analyse
the behavior of Ba.
(;3(5,0(176 24Na produced by KUCA reactor wasset on a p-type HPGe detector, GEM-35190S (ortec). The
gamma spectrum from 0 to 4 MeV was converted to 8192
ch digital data with an ADC (Multi-port II, Canberra). The
spectra were analysed using Gamma Explorer® software(Million Technologies). The source was placed on the axisof the detector at S–D distances (i.e., the distances fromthe surface of the end cap of the detector to the source),
which were varied from 0 cm to 10 cm. The measurement
time was set to collect more than 10,000 counts under thesum-peak area. Two peak counts, 1369 keV and 2754 keV,
the sum peak counts and the total counts were collected.
Also, 46Sc produced by KUCA reactor was measured as
the same way above. The peak, 889 keV and 1121 keV, thesum peak and the total counts were analysed. The angularcorrelation of the two peaks used here is 1.1184[5].
The behavior of Ba is trying to analysis. Radiobarium
produced by KUCA reactor was add to seawater sample.
Chemical separation procedure, using ion exchange or Sradsorbent, was performed and radiobarium in each fraction was analysed.
5(68/76 Fig. 1 shows the results of the sum-peakmethod and the modified sum-peak method applied to 24Na
analysis. The abscissa is the count rate of 1389 keV peak
and the ordinate is the estimated activity. The activities calculated with the sum-peak method and the modified sumpeak method were 2.83 kBq and 3.25 kBq, respectively.
The activities were somewhat different from the activity
calculated using efficiency at SDD 10 cm, 3.18 kBq, where
the sum peak effect was negligible. However, no reliable
figure of the angular correlation of the two peaks wasavailable. Therefore, the results cannot be verified. Contrary, the results of 46Sc are shown in Fig. 2. The calculated)LJ1DDQDO\VLVZLWKWKHVXPSHDNPHWKRGV)LJ6FDQDO\VLVZLWKWKHVXPSHDNPHWKRGV

activity by the modified sum-peak method were 26.6 kBq,
and the figure was a little bit smaller than the activity calculated from the data obtained at SDD 10 cm, 28.7 kBq.
The reason is now in investigation.
About the behavior of Ba, the limited results showedthat Ba was remain in the filter for both procedures. Therefore, just after the reactor accident, 140Ba was collected on
the filter. But the half-life of 140Ba is only 12.8 d, so thattree months after, the activity was less than two thousandth.
Therefore, the effect would be limited. And the increase of
the count brings conservative results. Moreover, the 140Ba
concentration will be estimated from the results by gamma
spectroscopy by HPGe.
More detailed analysis will be performed hereafter.
>@ K. Yuka HWDO,Proc. 19th Workshop on Environ. Radioact. KEK Proc. 2018-7, (2018)
>@ K. Yuka HWDO,Proc. 33th Workshop on Environ. Radiation Uses. KEK Proc. 2019-4, (2019)
>@ Y. Ogata HW DO, Nucl. Inst. Meth. Phys. Res. A. (2015)
>@ Y. Ogata HWDO, Appl. Radia. Isot.  (2016)
>@ G. BertoliniHWDO, Nuovo Cimento, 3 (1956)

31168

‑199‑

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E. Hibino, K. Morishima1, A. Okuda1, R. Inoue1, M.
Sugiyama1, and M. Nishimura

overall conformational change or not, we firstly analyzed
overall structural characteristics by MALDI-TOF/MS,
analytical ultracentrifuge (AUC) and SAXS.

0ROHFXODU1HXURVFLHQFH5HVHDUFK&HQWHU6KLJD8QLYHUVLW\RI0HGLFDO6FLHQFH
1,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\MonomerЎAIntensity (a.u.)

wild-type,1752'8&7,21 The number of patients with Alzheimer·s disease (AD) is increasing in Japan and AD isserious social issue. However, any effective ADmodifying drug is still undeveloped. The pathogenic
processes of AD are considered to be triggered by accumulation of amyloid-ǃ protein (Aǃ) in brain. Previously,
we have identified a secretory protein named interleukin-like epithelial-mesenchymal transition inducer (ILEI,
also known as FAM3 superfamily member C (FAM3C))
as a negative regulator of Aǃproduction by a novel activity1. ILEI is secreted from cell to bind to the extracellularregion of Presenilin-1, a component of the Ǆ-secretase
complex. The interaction of ILEI with Presenilin-1 enhances nonspecific degradation of Aǃ precursor protein.
ILEI was also reported ILEI C185A showed dysfunctionof tumor growth, and metastasis2. However, the relationship of Aǃ production inhibitory activity and tumor
growth and metastasis activity are still to be clarified.
The objective of this study is to elucidate struc- turefunction relationship that leads to develop a thera- peutic
drug for AD. We especially analyzed basic struc- turalcharacteristics of wild-type and C185A mutant of ILEI
and established experiment system.
(;3(5,0(176 Human wild-type ILEI and C185A
mutant (residues 55-227) with hexahistidine tag wereover-expressed in Rosetta-gamiB (DE3) pLysS stain andpurified by Ni-NTA resin and size exclusion chromatography (SEC). CBB-stained SDS-PAGE gels on non-redox
condition showed a single band.
For the MALDI-TOF/MS measurements, the purified
proteins were directly transferred onto the 96 spottedpolished steel target plate. After completely air drying,
the plate was loaded to the Microflex LT (Bruker Daltonics, Bremen, Germany). The spectra were generated inlinear positive ion mode.
For the structural characteristics, small-angle X-ray
scattering (SAXS) measurements of the purified proteinsat the concentrations of 1.0 mg/mL were performed withNANOPIX (Rigaku Corporation, Japan) at room temperature. The sample-to-detector distance and wavelength of
X-ray used for present work was 650 mm and 1.542 Å,
respectively. The scattering vector Tcovered from 0.02 to
0.3 Å-1.
5(68/76 We previously measured 2D-NMR spectra of wild-type and C185A 15N-ILEI. It was observed thepositions of around 20 peaks were changing (data notshown). To confirm whether the differences are caused by

C185A

B

Fig. 1. (A) MALDI-TOF/MS measurements of wildtype and C185A mutant of ILEI indicated molecular weights of monomer and multimers.
(B) Gunier plots obtained from the scattering curves.
in SAXS experiments.
The molecular weight of wild-type ILEI is around 20.0
kDa. The MALDI-TOF/MS measurements indicated thatno difference of abundance ratio of monomer and multimer between wild-type and C185A mutant (Fig. 1A). The
AUC experiments also supported the similar results (datanot shown).
Furthermore, to confirm overall structural differences
between wild-type and C185A mutant, SAXS experiments were conducted. From the Guinier analyzes of
SAXS profiles of wild-type and C185A mutant of ILEI,
no significant structural difference was observed between
them (Fig. 1B). Namely, C185A mutation did not affectto overall structure of ILEI.
Through these integrative experimental approaches, it
is expected that the NMR spectral change due to C185A
mutation is caused by the local structural change.
We have already had dysfunctional mutants for Aǃ
production inhibitory activity. We apply these analyticalmethods to these mutants for elucidation activity centerof ILEI.
5()(5(1&(6[1] H. Hasegawa HWDO., 1DW&RPPXQ, 5:3917 (2014)[2] M. Kral HWDO., )(%6-., 3484–3505 (2017)

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H. Yagi1, Y. Yunoki1,2, K. Morishima3, A. Matsumoto4, N.
Sato3, L. Porcar5, A. Martel5, R. Inoue3, H. Kono4, M.
Sugiyama3 and K. Kato1,2
*UDGXDWH6FKRRORI3KDUPDFHXWLFDO6FLHQFHV1DJR\D&LW\8QLYHUVLW\
([SORUDWRU\5HVHDUFK&HQWHURQ/LIHDQG/LYLQJ6\VWHPV1DWLRQDO,QVWLWXWHVRI1DWXUDO6FLHQFHV,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
1DWLRQDO,QVWLWXWHVIRU4XDQWXPDQG5DGLRORJLFDO6FL
HQFHDQG7HFKQRORJ\,QVWLWXW/DXH/DQJHYLQ
,1752'8&7,21  The molecular machinery of the
cyanobacterial circadian clock comprises three proteins:
KaiA, KaiB, and KaiC. Through interactions among thethree Kai proteins, the phosphorylation states of KaiC
generate circadian oscillations LQYLWUR in the presence ofadenosine triphosphate (ATP). We especially focused on
the KaiA-KaiB-KaiC ternary complex (ABC complex),
which is considered to play the key role of the negative
feedback loop of circadian rhythm. Recently, thecryo-electron microscopy (EM) structure of the ABC
complex has been reported. However, the N-domains of
KaiA subunits were poorly resolved due to their missing
electron density maps. This observation probably reflected a high flexibility of linker between N- andC-domains. The whole structure of ABC complex has
remained to be elucidated. Herein, for characterization of
the overall structure of ABC complex, we conducted integrative techniques using small-angle X-ray scattering(SAXS), inverse contrast-matching small-angle neutron
scattering (iCM-SANS), and native analytical ultracentrifugation (AUC) in conjunction with computer simulations.

(;3(5,0(176 The expression and purification ofclock proteins, KaiA, KaiB and KaiC were performed
according to methods previously described [1]. X-rays
from a high-brilliance point-focused X-ray generator(MicroMAX-007HF, Rigaku, Tokyo, Japan) were focused with a confocal mirror (OptiSAXS) and collimatedwith a confocal multilayer mirror and two pinholes collimation system with the lower parasitic scattering,“ClearPinhole”. The scattered X-rays were detected witha two-dimensional semiconductor detector (HyPix-6000,
Rigaku, Tokyo, Japan). The sample-to-detector distanceand wavelength of X-ray used for present work was 1320
mm and 1.542 Å, respectively. For removal of unfavorable aggregates from the sample solution, the laboratory-based SEC-SAXS System (LA-SSS) was employed tomeasure the SAXS profile in the 4 range (0.01Å-1–0.2Å-1). The SANS experiments were performed
using the D22 instrument installed at the Institut
Laue-Langevin (ILL), Grenoble, France. The sample-to-detector distance and wavelength of neutron used

for present work was 5600 mm and 6.0 Å, respectively.
SEC-SANS system was also utilized for present work.
5(68/76 The AUC data confirmed that KaiA, KaiB,
and KaiC formed a 12:6:6 complex under the excess
amount of KaiA.
With the aid of La-SSS, we succeeded to obtainmono-disperse ABC complex SAXS data. To obtain the
structural information of subunits in the ABC complex in
more detail, we also utilized the SEC-iCM-SANS. In thisstudy, we prepared the ABC complex consisting of the
75% deuterated KaiB and KaiC subunits and the nondeuterated KaiA subunits. The solvent D2O ratio at thecontrast matching point was determined to eliminate
scattering originating from the 75% deuterated KaiC
subunits. As a result, we could exclusively observe the
SANS profile from KaiA subunits in the complex.
Under the assumption of six-fold symmetry of arrangement of the 12 KaiA N-domain connected with EM
structure of ABC complex, we made 20 million distinct
structural models of the ABC complex. The SAXS andSANS scattering profiles were calculated for each modeland compared with the experimental data. As shown in
Fig. 1, the whole structure of ABC complex as well as the
structural arrangement of the KaiA-N-domains in thecomplex was resolved.
In summary, we succeeded to solve the ABC complex
structure using SEC-SAXS and SEC-SANS in conjunction with computer simulation. Present result should provide the insights into the working mechanisms of the circadian clock comprised of Kai proteins.
  
 



 

Fig. 1Structural model of
KaiA-KaiB-KaiC
complex based on
the scattering data.
N- and C-domainsof KaiA, KaiB and
KaiC are shown ingreen, blue, redand gray, respectively.

5()(5(1&(6[1] M. Sugiyama HWDO, Si. Rep., _(2016).

31006
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R. Maeda, S. Nagatoishi1, K. Tsumoto1, K. Morishima2,
R. Inoue2, M. Sugiyama2 and M. Hoshino*UDGXDWH6FKRRORI3KDUPDFHXWLFDO6FLHQFHV.\RWR
8QLYHUVLW\,QVWLWXWHRI0HGLFDO6FLHQFHWKH8QLYHUVLW\RI7RN\R,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Oxygen is essential for many organisms to produce ATP efficiently from nutrients infood. Under the normal oxidative conditions, nutrientsare metabolized through glycolytic pathway, tricarboxyl-ic
acid cycle and electron transport system. Temporal or
local drop of oxygen level induces cells to change themetabolic pathway, which is known as hypoxia stressresponses. The responses are mainly triggered by hypoxia inducible factors (HIFs) that activate transcriptionof a group of genes.
Under the normal oxygen conditions, transcriptional
activities of HIFs in the cells are inhibited by the factor
inhibiting HIF-1 (FIH-1). On the other hand, several
cells including tumor cells and macrophages, metabolize
nutrients exclusively by nonoxidative glycolytic pathway
even under the normal oxygen levels. Munc-18 interacting protein 3 (Mint3) is recently found to activate thehypoxia responses by binding and inhibiting the activityof FIH-1 in these cells [1]. Although the N-terminal
214 residues are found to be necessary for the interaction
with FIH-1 to inhibit its activity, little is known about
inhibitory mechanisms.
We attempted to elucidate the molecular mechanismof the interaction between Mint3 and FIH-1 by a various
physicochemical methods, including small-angle X-ray
scattering, analytical ultracentrifugation, and solution-state NMR.

5(68/76 We measured 1H-15N HSQC spectra of
Mint3(1–214) and Mint3(1–117) proteins under thephysiological conditions (pH 7.3). In both proteins, thechemical shift dispersion along the 1H axis was small andmost peaks were appeared within the range between 8.5
and 7.5 ppm, suggesting that the proteins were intrinsically disordered. This was also supported by the obser that the peak intensities were markedly decreased
vationat higher temperature, probably rapid exchange of amidehydrogen with water molecules due to the lost of intramolecular hydrogen bonds.
Next, we measured the 1H-15N HSQC spectra of
Mint3(1–214) and Mint3(1–117) in the presence of avarious amount of unlabeled FIH-1. In both proteins,the intensities for several peaks were markedly decreased
in a concentration-dependent manner, suggesting the involvement of specific binding of these residues. It
should be mentioned that the same results were obtained
both in Mint3(1–214) and Mint3(1–117), suggesting thatthe specific binding site for FIH-1 is present in a smaller
fragment protein Mint3(1–117) (Fig. 1).

Fig. 1 1H-15N HSQC spectra of Mint3(1–117) in theabsence (left) and presence (right) of unlabeled
FIH-1.

(;3(5,0(176High-expression systems for the
N-terminal fragment proteins of Mint3 (Mint3(1–214)
and Mint3(1–117)) and full-length FIH-1 were constructed by E. coli BL21 strains. The proteins were exIn order to elucidate the binding site at residue-level,pressed in bacteria grown in LB-broth and 15N-enriched we are now analyzing several 3D-triple resonanceM9 minimal medium to produce unlabeled and experiments, including 3D-HNCACB and 3D-hNcocaNH,
15
to assign the resonance peaks. We are also attempting
N-labeled proteins, respectively.
NMR experiments were performed on a Bruker to analyze global change in the molecular shape of
Avance 600 spectrometer equipped with a tri- Mint3(1–214) / Mint3(1–117) and FIH-1 by small-angle
ple-resonance probe. A typical 1H-15N HSQC experi- X-ray scattering.
ments were performed at protein concentration of 50 μM.
The solvent conditions used were 20 mM sodium acetate(pH 7.3), and 10% D2O. The chemical shift value was 5()(5(1&(6[1] Sakamoto et al. (2014) Mol Cell Biol. 34 (1) 30–42.
referenced to DSS.

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6XSUDPROHFXODU7KRORV/LNH$UFKLWHFWXUH&RQVWLWXWHGE\$UFKDHDO3URWHLQV:LWKRXW)XQFWLRQDO$QQRWDWLRQ

M. Yagi-Utsumi, R. Inoue1, M. Sugiyama1 and K. Kato([SORUDWRU\5HVHDUFK&HQWHUIRU/LIHDQG/LYLQJ6\VWHPV([&(//6 DQG,QVWLWXWHIRU0ROHFXODU6FLHQFH ,06 
1DWLRQDO,QVWLWXWHVRI1DWXUDO6FLHQFHV,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 Euryarchaeal genomes encode
proteasome-assembling chaperone homologs, PbaA and
PbaB, although archaeal proteasome formation is a chaperone-independent process. Homotetrameric PbaB functions as a proteasome activator, while PbaA forms ahomopentamer that does not interact with the proteasome[1, 2]. Notably, PbaA forms a complex with PF0014, anarchaeal protein without functional annotation. In thisstudy, based on our previous research on PbaA crystal
structure, we performed an integrative analysis of thesupramolecular structure of the PbaA/PF0014 complex
using native mass spectrometry, solution scattering,high-speed atomic force microscopy (HS-AFM), andcryo electron microscopy (cryo-EM).
(;3(5,0(176 For the purification of the
PbaA/PF0014 complex, both recombinant proteins, PbaA
(400 μM monomer) and PF0014 (400 μM monomer),
were mixed at a 1:1 molar ratio and then dialyzed for
12 h against 50 mM Tris–HCl buffer (pH 8.0) containing
200 mM NaCl and 2 mM DTT.
SEC-SAXS measurements of the PbaA/PF0014 complex were obtained using UPLC ACQUITY (Waters) integrated with a SAXS set-up. In each measurement,
50 μL of 6 mg/ml proteins was loaded onto a Superdex
200 Increase 10/300 GL (GE Healthcare) pre-equilibrated
with 50 mM Tris–HCl buffer (pH 8.0) containing
150 mM NaCl at a flow rate of 0.5 ml/min. During theelution of proteins, the flow rate was reduced to0.10 ml/min. X-ray scattering and UV spectra were collected every 10 s.
For iCM-SANS experiments, a complex of 3 mg/ml of
non-deuterated PbaA/75%-deuterated PF0014 as well as
a complex of 75%-deuterated PbaA/75%-deuterated
PF0014 was dissolved in 99.8% D2O (ISOTEC) containing 50 mM Tris–HCl (pH 8.0) and 150 mM NaCl to reduce the incoherent scattering and obtain high-quality
statistical data in the higher q-range. SANS experiments
were performed using Quokka installed at the Australian
Centre for Neutron Scattering (ANSTO, Sydney, Australia).

iCM-SANS, cryo-EM, and HS-AFM showed that two
PbaA homopentameric rings correspond to the dumbbell
plates, with their N-termini located outside of the plates
and C-terminal segments left mobile. Furthermore, mutant PbaA lacking the mobile C-terminal segment retained the ability to form a complex with PF0014, allowing 3D modeling of the complex. The complex shows afive-column tholos-like architecture, in which each column comprises homodimeric PF0014, harboring a central
cavity, which can potentially accommodate biomacromolecules including proteins. Our findings provide insight into the functional roles of Pba family proteins, offering a novel framework for designing functional protein
cages [3].

Fig. 1. (A) The SEC chart of the PbaA/PF0014
complex. We selected a region of full width at half
maximum of the main peak from W = 2664 to W =2900 s, indicated by red lines, for averaging the
SAXS profile. (B) Averaged scattering profile. (C)Guinier plot indicating the range for the least square
fitting by arrows and (D) distance distribution function, 3(U), of the averaged SAXS profile.

5()(5(1&(6[1] A. Sikdar HW DO, Biochem. Biophys. Res. Commun.,(2014) 493-497.
[2] M. Yagi-Utsumi HW DO, Protein. Eng. Des. Sel., (2018) 29-36.
[3] M. Yagi-Utsumi, HWDO, Sci. Rep, , (2020) 1540.

5(68/76 The results indicated that this highly thermostable complex constitutes ten PbaA and ten PF0014
molecules, which are assembled into a dumbbell-shaped
structure. SEC-SAXS showed the PbaA-PF0014 complex
exhibits an estimated radius of gyration (5g) of 54.6̳cand maximum dimension ('max) of 165 ̳ c (Fig. 1).

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Small Angle X-ray Scattering Measurements on Insulin B-Chain
Nucleation Intermediate Complexed with FibrinogenN. Yamamoto, E. Chatani1, T. Akai1, R. Inoue2and M.
Sugiyama2

the length was approximately 270 nm based onBroersma’s relationship [4] with a diffusion coefficient determined by DLS measurement. The rod-like structure wasmaintained even after the addition of fibrinogen, and theslope of the log-log plot kept close to -1. When the baseradius and length of the complex were calculated in thesame manner as for the nucleation intermediate, they were
estimated to be 6 nm and 290 nm, respectively [5].

School of Medicine, Jichi Medical University
1
Graduate School of Science, Kobe University
2
Institute for Integrated Radiation and Nuclear Science,
Kyoto University

4

10

INTRODUCTION: Amyloid fibrils are protein aggregates with β-sheet rich structure, which are associated withnumerous amyloidoses and neurodegenerative diseases.
Amyloid fibrils are typically formed through a nucleationdependent mechanism. While a one-step nucleation is thesimplest scheme, various oligomers have been identifiedin early stages, suggesting the presence of meta-stable nucleation intermediates [1].
In our previous work, we found that nucleation intermediates were formed in the early phases of amyloid fibril
formation of an insulin-derived peptide, insulin B chain[2]. In addition, we found that fibrinogen, one of dominant
plasma proteins, inhibits the formation of amyloid fibrils
of insulin B chain by interacting with nucleation intermediates [3]. In this study, we elucidated structural propertiesof the nucleation intermediate by using small-angle X-ray
scattering (SAXS) and analyzed change in SAXS profile
after the addition of fibrinogen to elucidate the interaction
manner of fibrinogen with the nucleation intermediate.

nucleation intermediate
fibrinogennucleation intermediate + fibrinogen

3

10

-3

I(q) /10 ·cm

-1

2

10

1

-1

10

-2

0

10

-4
-1

10

6 7 89

0.01

2

3

4

q /A

5 6 7 89
-1

0.1

2

Fig. 1. One-dimensional SAXS profiles of the nucleation intermediate of insulin B chain (black), fibrinogen(orange) and the complex of the nucleation intermediate
and fibrinogen (blue). Gray lines represent the slope of
the profiles and the black slopes of -1, -2, or -4 indicate
guides for the eyes.

EXPERIMENTS: B chain was prepared from humaninsulin as described in a previous work [2]. The stock insulin B chain was diluted with 50 mM Tris-HCl buffer at
a concentration of 1.4 mg/ml and was then put in a 1-mm
path-length quartz cell. For the measurement of the Bchain nucleation intermediate, the sample was pre-incubated under quiescent conditions for 2 h at 25 °C. For themeasurement of the complex with fibrinogen, a concentrated fibrinogen solution was added to the nucleation intermediate at the final concentration of 3.5 mg/ml approximately 5 min before the SAXS measurement. For themeasurement of fibrinogen, a 3.5 mg/ml solution in 50
mM Tris-HCl buffer was used. SAXS profiles were measured at 25 °C with NANOPIX equipped with HyPix-6000(Rigaku Corporation, Japan) with an exposure time of 30
min. A Cu K-α line (MicroMAX-007HF) was used as abeam source. The camera length was 1.33 m and the rangeof the scattering vector q was from 0.006 to 0.23 Å-1.

The radius of fibrinogen was approximately 2.5 nm,
and the increase in the radius by the fibrinogen binding
could be explained reasonably when a single layer of fibrinogen molecules was assumed to surround the surfaceof the prefibrillar intermediates. It was thus suggested thatfibrinogen binds to the surface of the nucleation intermediate so as to cover the surface of the nucleation intermediate, which would be the molecular basis of the inhibitory
mechanism of B-chain amyloid fibril formation by fibrinogen. This structural insight of the B-chain nucleation intermediate complexed with fibrinogen will provide insights into general principles of functions of proteins thatserve as chaperones or chaperone-like proteins involved inamyloid-related diseases.

RESULTS: Figure 1 shows the SAXS profile of the Bchain nucleation intermediate, fibrinogen, and the complex of the nucleation intermediate with fibrinogen. The
slope of the log-log plot of the scattering profile of the nucleation intermediate was close to -1, suggesting a rod-likestructure. As a result of the analysis of a cross-section plot
for a cylindrical structure, it was suggested that the bottom
radius is approximately 3 nm. It was also suggested that

REFERENCES:[1] E. Chatani and N. Yamamoto, Biophys. Rev., 10 (2018)527-534.
[2] N. Yamamoto et al., Sci. Rep., 8 (2018) 62.
[3] T. Akai, Master’s Thesis, Kobe Univ. (2017).
[4] S. J. Broersma, Chem. Phys., 32 (1960) 1632-1635.
[5] N. Yamamoto et al., Biochemistry, 58 (2019) 27692781.

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H. Terato, T. Saito1, Y. Sakurai1, T. Hanafusa, M. Isobe,
S. Ihara2 and Y. Tokuyama3$GYDQFHG6FLHQFH5HVHDUFK&HQWHU2ND\DPD8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ6DJD8QLYHUVLW\
$QDO\WLFDO5HVHDUFK&HQWHUIRU([SHULPHQWDO6FLHQFHV
6DJD8QLYHUVLW\,1752'8&7,21  Radiation biological effects arearrived via DNA damaging by ionizing radiation, because
DNA brings the genetic information. We have a lot ofknowledge about radiation DNA damage. But the most ofthem were derived from gamma- and X-rays’ studies withless information of other radiation qualities. Therefore,
we have studied for the DNA damage with heavy ion
beams, previously [1, 2]. These studies indicated that the
DNA damage with heavy ion beams were unique,indicating that a lot of clustered DNA damage weregenerated including DNA double strand break (DSB),
clustered base lesions, and these mixtures. Clustered
DNA damage is a complex damage containing multiple
lesions in the local region of DNA. This damage strongly
inhibits DNA polymerization with high efficiently
stopping of DNA polymerase moving on DNA. Also,
clustered DNA damage shows less repairable, because
there is no scaffold for DNA repair enzyme attaching.
Here, we analyze the DNA damage with neutrons from
nuclear power plant to unveil the molecular mechanismof neutron biological effect. The neutron beam is alsohigh LET radiation as same as heavy ion beam. Therefore,
we will find some interesting character of DNA damage
with neutron like heavy ion beam. In the previous study
period, we found the relatively higher yields of DNA
damage with the neutron beams than gamma-rays. In thisyear, we estimated the cell viability for the neutron beams
for the biological effect of this radiation.
(;3(5,0(176 Cultured cells of Chinese hamster
ovary (CHO) AA8 strain were irradiated with neutron
beams in the Kyoto University Reactor. The cells were
cultivated with the conventional method. The logarithmic
growing cells were recovered by trypsinization, and set
into a polypropylene tube for irradiation. The irradiation
time was up to three hours with sampling in every 30
minutes. The estimated dose rate of neutron was 1Gy h-1.
After irradiation, the cells were immediately dissolved
again with the cultured medium and reseeded into fresh
medium. The cells were cultivated for 10 days for
growing the colony. The colony was fixed with ethanoland stained with methylene blue. The colony number wascounted for estimation of the irradiated cell viability.

5(68/76 The result for cell viability indicated thatneutron showed stronger cell damage ability than
gamma-rays (Fig. 1). The surviving curve indicates that
D37 of the neutron seems to be around 1 Gy. The
dosimetry of the neutrons indicates that a half of dose of
the reactor neutrons is derived from the contaminatedgamma-rays (data not shown). Gamma-rays usually showthat the D37 is around 4 Gy. This result suggests that theneutron has greater efficiency for the biological effect.
We already have the result indicating that the neutron
showed relatively higher efficiency to generate the DNA
damage than gamma-rays. Thus, the severe biologicaleffect with neutron beam seems to be derived from thehigher yield of DNA damage.
In this yearly study, we obtained the relatively higher
biological effect of the neutron. But, we need further
study for elucidation of molecular mechanism of neutron
biological effect. The first one is generalization ofneutron effect. We are proceeding another neutron projectat Kinki University Reactor (KUR). KUR generates
weaker power neutron than the Kyoto University reactor.
Comparing of the results with these two reactors willshow a generalization of neutron efficiency. The second
is analysis of DNA damage species with neutron beam.
The future analyzing plan will contain the oxidative
pyrimidine analysis such as 5-hydrooxycytosine. Also,
the DSB will be analyzed by using of the mutant cellstrains without homologous recombination (HR) andhon-homologous end joining (NHEJ). Using of thesemutants leads the initial yields of DSB without DNA
repair process.

Fig. 1. Surviving fraction of the cells irradiatedwith the reactor neutrons.

5()(5(1&(6>@ H. Terato et al., J. Radiat. Res., 49 (2008) 133-146.
>@ Y. Tokuyama et al., J. Radiat. Res., 56 (2015) 446-455.

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K. Akamatsu, N. Shikazono and T. Saito

nol-precipitation followed by ultrafiltration. The fluorescence anisotropy was measured at 525 nm (ex. 470 nm).
The anisotropy, < U >, is defined as follows:,QVWLWXWHRI4XDQWXP/LIH6FLHQFH1DWLRQDO,QVWLWXWHVIRU
4XDQWXPDQG5DGLRORJLFDO6FLHQFHDQG7HFKQRORJ\
467 < U > = (,99 – *,9+ ) / (,99 + 2*,9+ ),



.8516

,1752'8&7,21DNA lesions induced by ionizing radiation andchemicals can cause mutation and carcinogenesis. In
particular, “clustered damage” site, that is a DNA region
with multiple lesions within one or two helical turns, isbelieved to hardly be repaired. This damage is considered
to be induced, HJ, around high-LET ionizing radiation
tracks In fact, evidence is found in the direct observation
AFM (atomic force microscopy) and a simulation [1].
However, detail of the damage is not known. We havealready developed a method for estimating degree of
localization of abasic sites (APs) in DNA using F|rster
resonance energy transfer occurred between different
fluorescence probes (“hetero-FRET” using Alexa350 andAlexa488) [2]. The results showed that 12C5+ beam produced close APs within a track: the apparent distancecalculated was approximately 17 base pairs [3]. Thisfinding indicates that direct radiation effect of 12C5+ beamnear the Bragg peak produces clustered DNA damage.
We have recently applied the method to DNA in acell-mimetic radical scavenging condition. However,there are some problems of the complex protocol and of
the sensitivity due to the low extinction coefficient of
Alexa350. We have, therefore, developed “homo-FRET”
occurred between two or more Alexa488 molecules. We
will obtain magnitude of FRET also from “fluorescenceanisotropy” of homo-FRET between Alexa488 molecules.
The new protocol using homo-FRET [4] enables us toestimate DNA damage localization without any enzymes
and improves sensitivity to detect a clustered damage.

where ,99 is the fluorescence intensity when the excitation and emission polarizers are both vertically oriented.
,9+ is one when the excitation/emission polarizers arevertically/horizontally oriented. * is the grating factor
defined as ,+9/,++.
5(68/76$1'',6&866,21

(;3(5,0(176
Ɣ6DPSOHSUHSDUDWLRQDQGLUUDGLDWLRQ
The plasmid DNA digested by Sma I was used (linear
form). The DNA was dissolved to be ~10 mg/mL in 0.2
M Tris-HCl buffer (pH 7.5) which is a cell-mimetic condition in relation to radical scavenging capacity. Eightmicroliters of the DNA solution was transferred to a glass
plate (10 mmI) under 100 % RH at r.t., and was irradiated with heavy ion beams, 20Ne8+ (LET: ~500 keV/Pm),
40
Ar13+ (LET: ~1800 keV/Pm) at TIARA (QST), and 60Co
J-rays (LET: ~0.3 keV/Pm; KURNS) as a standard radiation source.
Ɣ3UHSDUDWLRQRIIOXRURSKRUHODEHOHGLUUDGLDWHG'1$DQG
WKH)5(7REVHUYDWLRQ
The damaged sample DNA (10 PL in water) and 10
PL of 100 mM Tris-HCl (pH 7.5) were mixed in a microtube. Two microliters of Alexa488/DMSO was added
to the DNA solution and was incubated for 24 h at 35C.
The fluorophore-labeled DNA was purified by etha-



‑208‑

Fig. 1. Relationship between AP averaged density and fluorecenceanisotropy for 60Co J-rays (ŏ), Ne (ʆ), and Ar (ʄ). The solid line indicates a theoretical curve when APs are randomly distributed.

In general, fluorescence anisotropy decreases withincreasing FRET [5]. As shown in Fig.1, we found thatthe relationship differed significantly among the radiations tested. AP clustering even by the J-rays seems to
be more likely to occur than random distribution. Although the ion beams appeared to produce clustered AP
more than the case of the J-rays, the difference was not
so significant that we expected from the results for the
direct radiation effects using dry DNA samples [3].
Under cell-mimetic condition, most APs induced by theion beams could exist as isolated lesions. Production ofclustered APs by “indirect effect” (HJ, by yOH) may
hardly occur due to recombination between radicals.
5()(5(1&(6>@ Y. Matsuya, HWDO, Int.J.Mol. Sci. 20, 1701.
>@ K. Akamatsu, N. Shikazono, Anal. Biochem. (2013) 171-180.
>@ K. Akamatsu, N. Shikazono, and T. Saito, Radiat.
Res. (2015) 105-113.
>@ K. Akamatsu, N. Shikazono, Anal. Biochem. (2017) 78-89.
>@ L. W. Runnels, and S. F. Scarlata, Biophys. J. (1995) 1569.

&23KRWRSURGXFWLRQRI0HGLFDO)DQG P7F,VRWRSHV

M. Kurosawa 1, M. Fujiwara 1, N. Takahashi1,2 ,M. Tamura 1, Y. Kosuge 2, N. Abe 3 , T. Kubota 3 , and T.
Takahashi3

to develop the new method for extracting 99mTc using
nano-particles.

1 5HVHDUFK&HQWHUIRU1XFOHDU3K\VLFV 2VDND8QLYHUVLW\
2 .\RWR0HGLFDO7HFKQRORJ\&R
3 ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21In the 18 F production, we use natural neon gas as a target
in the gas recycling flow system. The 18 F-FDG pharmaceuticals are obtained by blowing small bubbles of irradiated neon gas in the glucose aqueous solution. In the 99mTc
production, we use natural MoO3 . In both the methods, we
can produce 99mTc isotopes for the SPECT inspections and
18 F isotopes for the PET inspections using the photoreaction on natural MoO3 and Ne targets. We are going topolish up the usages of these two methods in view of practical aspect. .
 )(;3(5,0(17$1'5(68/76

An electron beam from the linear accelerator facility at
Institute for Integrated Radiation and Nuclear Science of
Kyoto University (KURNS-LINAC) for producing RIfrom photoreactions. A 40 MeV electron beams with anintensity of 3-9 PA is used to bombard a platinum target
with a thickness of 4 mm to generate bremsstrahlung photons for producing 18 F via the photoreaction on natural Ne
gas.
7KH1HJDVFLUFXODWLRQV\VWHPKDVEHHQGHYHORSHG
IRUWKHSUHVHQWH[SHULPHQW7KHLUUDGLDWLRQWLPHRIEUHPVVWUDKOXQJSKRWRQVZDVRQHKRXU:HH[SHFWWKDWSURGXFHG)LVRWRSHVFLUFXODWHZLWK1HJDV
DQG WKDW WKH PRQRYDOHQW2+ LQ JOXFRVHZLOO EH
HDVLO\ UHSODFHGE\) DUUHVWHGLQ WKHOLTXLG UHVXOWLQJ)'*7KHILUVWSXUSRVHRIWKHH[SHULPHQWZDVWRH[DPLQHWKLVSULQFLSOH,QVWHDGRIJOXFRVH
ZHXVHGDVRGLXPK\GUR[LGH 1D2+ DTXHRXVVROXWLRQWRWUDS )7KLVVHHPHGWREHVXFFHVVIXOLQ)FROOHFWLRQ+RZHYHUZKHQZHXVHGJOXFRVHLQVWHDGRI1D2+
the 18F collection efficiency drastically decreased. The
clear reason is still unknown. The reasons may come from
1) the intrinsic easiness of the chemical replacement reaction for the glucose and NaOH.
 P7F(;3(5,0(17$1'5(68/76

It had been reported that the high-rate production of
99m Tc radioisotopes is realized by irradiating the bremsstrahlung photons on natural MoO3 target [1,2]. We tried

Figure 1: Photoreaction produces 99Mo in nano-MoO3 powderwhich has a porous assembly of many MoO 3. 99mTc radioisotopes
decayed from 99Mo are washed out using saline.

Figure 1 shows the schematics scheme for producing
99m Tc via the 100 Mo(J,n) 99Mo reaction. We notice that thesize of the nano-particles is very small and the most of the
99 Mo produced by the photo-nuclear reaction can escapeto the surface. Therefore, the produced 99mTc is easily separated from the natMO3. If we pour the isotonic sodium
chloride solution (saline) into nano-MoO3 powder, 99mTc isreadly soluble in saline even at the inside of nano-particles.

Figure 2:-ray spectrum measured with a Ge-detector after

99mTc separation using saline. Two prominent-ray peaks at
140.5 keV from 99mTc and at 1460.9 keV from 40K as backgroundare measured. The event yields lower than 140.5 keV are due to
X-ray background from Pb shields and due to the Compton scattering of 140.5 keV J-ray.

Figure 2 shows aJ-ray spectrum measured for the saline
leaked out from the target vessel of MoO3 nano-powder.
Although we observe the backgrounds due to the X-rays
from Pb-shields and due to the 1460.9 keVJ-ray from 40K,
it is clear that the saline leaked out from the target vessel
includes only 99mTc (see the 140.5 keV peak).
5()(5(1&(6>@ T. Takeda HWDO, 99mTc production via the (γ,n) reaction
on natural Mo, Journal of Radioanalytical and Nuclear
Chemistry (2018) 318: 811-821.
>@ N. Takahashi, Patent Number 2014/05790

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&2

6PDOO$QJOH;UD\6FDWWHULQJ0HDVXUHPHQWVRQ,QVXOLQ%FKDLQD7LPH5HVROYHG
0HDVXUHPHQWWR0RQLWRUWKH$P\ORLG)LEULO)RUPDWLRQYLD3UHILEULOODU,QWHUPHGLDWHV

N. Yamamoto, R. Inoue1, K. Morishima1, E. Chatani2,and M. Sugiyama1

and the range of the scattering vector T was from 0.05 to
2.35 nm-1. X-ray scattering data were collected with an
exposure time of 30 min.

6FKRRORI0HGLFLQH-LFKL0HGLFDO8QLYHUVLW\,QVWLWXWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\2*UDGXDWH6FKRRORI6FLHQFH.REH8QLYHUVLW\,1752'8&7,21  Amyloid fibrils are abnormal
protein aggregates associated with a numerous number of
diseases called amyloidoses such as Alzheimer’s disease.
Amyloid fibrils generally possess fibrous morphology
and ȕ-sheet-rich structure, and the formation of amyloid
fibrils typically follows a nucleation-dependent polymerization mechanism. It has been believed that the fibril
formation occurs by one-step reaction from fibril nuclei.
However, a variety of oligomers have been identified inearly stages of fibrillation. Such oligomeric species attract attention as a key molecule in the nucleation process
as well as molecular species responsible for cytotoxicity[1].
We recently found that prefibrillar intermediates wereformed in the early phases of amyloid fibril formation of
an insulin-derived peptide (insulin B chain) [2]. Especially, it was confirmed that two kinds of prefibrillar intermediates, i.e. the first prefibrillar intermediate and thesubsequently-occurring second prefibrillar intermediate
were formed. The structural detail of prefibrillar intermediates was elucidated using time-resolved small-angle
X-ray scattering (SAXS) at the concentration of 1.4
mg/ml [3]. The analysis of the time-resolved measurement suggested elongation of the rod-like structure as thenumber of the second prefibrillar intermediate increased.
In this study, we also performed time-resolved SAXS
experiment at the B chain concentration of 2.8 mg/ml tounderstand more detail about the elongation mechanismof the prefibrillar intermediates toward the fibril formation.
(;3(5,0(176 For the purification of B chain fromhuman insulin, we followed the purification method of B
chain described in literature [4]. The stock insulin B
chain, which was dissolved in 10 mM NaOH, was diluted
with 50 mM Tris-HCl buffer at a concentration of 2.8
mg/ml. The sample solution was then put in a 1-mm
path-length quartz cell. SAXS profile was obtained at
25 °C with NANOPIX equipped with HyPix-6000(Rigaku Corporation, Japan). A Cu K-Į OLQH (MicroMAX-007HF) was used as a beam source, which was
further focused and collimated with a confocal multilayer
mirror (OptiSAXS). The camera length was set to 1.33 m

5(68/76 Fig. 1 shows time-resolved SAXS profilesof insulin B chain at the concentration of 2.8 mg/ml. It
was demonstrated that the slope of the plot in the double-logarithmic scale was close to -1, indicating that theintermediates possess rod-like structures. A preliminary
analysis of the cross-section plot, in which the intensity
was plotted against T2, was also performed to calculate
the radius of the rod-like structure. As a result, it wasdemonstrated that the first prefibrillar intermediate wasalready formed even in the dead time of the measurement.
It indicates that the increase in the concentration accelerated the formation of the first prefibrillar intermediate.
Combined with a result of time-resolved dynamic lightscattering measurement, it was also revealed that further
elongation of the second prefibrillar intermediate occurred. This behavior supports our proposed idea that theformation of the amyloid fibril occurs via the second
prefibrillar intermediate.

Fig. 1. Representative one-dimensional SAXS profiles of insulin B chain monitored at 20, 110,
and 1,220 minutes. The lines indicate slopes
obtained by curve Iit.

5()(5(1&(6>@ E. Chatani and N. Yamamoto, Biophys. Rev., (2018) 527-534.
>@ N. Yamamoto HWDO., Sci. Rep.,  (2018) 62.
>@ N. Yamamoto HW DO., KURNS PROGRESS REPORT
2018, CO6-7 (2018).
>@ N. Yamamoto HW DO Biochemistry, 58 (2019)2769-2781.

31070

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Generation of radioresistant Escherichia coli by adaptive evolution
using gamma rays as selection pressure II

T. Saito
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: In nature, organisms have evolved
diversely by adapting themselves to various environmental
conditions. Some organisms have been found to survive inenvironments that can be easily perceived as extremely severe. Elucidating the adaptive mechanisms of organisms
to severe environmental conditions can provide meaningful information regarding evolution and diversity overall.
Some bacteria, known as radioresistant bacteria, demonstrate extreme resistance to ionizing radiations [1]. The extreme resistance mechanism of these bacteria to ionizing
radiation is an interesting area of research from the standpoint of adaptive mechanisms employed by organisms innature. In order to elucidate the mechanisms of radioresistance in these organisms, it is important to investigate
their biological defense mechanisms against external
stresses at the molecular level. However, studies conducted on radioresistant organisms existing in nature arelikely to encounter many challenges due to limited
knowledge of their genetic and biochemical properties.
Therefore, in this study, the generation of radioresistantcells of Escherichia coli was attempted by experimenting
on their ability to undergo adaptive evolution when exposed to gamma rays. The following operations were repeated in this experiment: gamma-ray irradiation of E. coli
cells whose genetic and biochemical properties are sufficiently known, growth of the surviving cells, and irradiation of the grown cells. Furthermore, the gene expression
status in evolved E. coli was analyzed and compared withthat of wild type E. coli.
EXPERIMENTS: Evaluation of the sensitivity of E.
coli cells to gamma irradiation: E. coli K-12 cells weregrown to the early log phase in LB medium at 37°C at 200rpm. One milliliter of the culture was centrifuged at 4000
× g at 20°C for 10 min. The supernatant was discarded andthe pellet was suspended in 1 mL of PBS (–). The cell suspension was irradiated with gamma rays at a dose rate of
22 Gy/min at 20 ± 3°C. Gamma irradiation was carried out
at the Co-60 Gamma-ray Irradiation Facility of the Institute for Integrated Radiation and Nuclear Science, Kyoto
University. The gamma-irradiated cell suspension was diluted appropriately with PBS (–), plated on LB agar, andincubated at 37°C for 12 hr. After incubation, the colonies
were counted, colony forming units were determined, andsurvival rates were calculated.
Selection with gamma rays: E. coli K-12 clone cells

obtained by single colony pick-up were cultured to theearly log phase in LB medium at 37°C at 200 rpm. The cellsuspension was prepared as described above and irradiatedwith the 1% survival dose of gamma rays at a dose rate of
22 Gy/min at 20 ± 3°C. One milliliter of the gamma-irradiated cell suspension was inoculated in 100 mL of LB
medium and cultured at 37°C at 200 rpm till the cells
reached their early stationary phase. The glycerol stock
was prepared and stored at –80°C. This procedure was repeated after culturing the glycerol stock cells to the earlylog phase.
Analysis of gene expression status  Total RNA wasextracted from E. coli cells using RNAiso Plus (Takara),
and further purified using NucleoSpin RNA Clean-up XS(Macherey-Nagel). The quality of the resulting total RNA
was evaluated and confirmed with the Agilent 2200
TapeStation (Agilent). rRNA was removed from total
RNA using Ribo-Zero Magnetic Kit (Gram-Negative
Bacteria) (Illumina). The sequence library was preparedfrom the resulting RNA using TruSeq Stranded mRNA
Sample Prep Kit (Illumina). The quality of the sequencelibrary was evaluated and confirmed with the Agilent 2100
Bioanalyzer (Agilent). Sequence analysis was performed
with NovaSeq 6000 (Illumina) and using NovaSeq 6000
S4 Reagent Kit (Illumina) and NovaSeq Xp 4-Lane Kit (Illumina). The gene expression levels were analyzed using
Genedata Profiler Genome (Genedata) and STAR [2]. Allprocedures were done according to manufacturer's instructions.
RESULTS: The 1% survival dose to gamma rays of thewild type E. coli clone without selection was 240 Gy,
whereas that of the E. coli population obtained after 20 selection cycles was 1900 Gy; the resistance of E. coli to
gamma rays was increased 7.9-fold in this adaptive evolution experiment. The expression levels of 164 genes in the
evolved E. coli were statistically significantly different
from those in the wild-type E. coli. Among those genes,
the expression level of 27 genes increased 2-fold or more,
and the expression level of 23 genes decreased 0.5-fold or
less. These results suggest that the radioresistance of theradioresistant E. coli obtained in this adaptive evolution
experiment is attributed in part to these genetic changes.
In the future, it is necessary to analyze in detail how thesechanges in gene expression are involved in theradioresistance of E. coli.
REFERENCES:[1] T. Saito, Viva Origino, 30 (2007) 85–92.
[2] A. Dobin et al., Bioinfomatics, 29 (2013) 15–21.

31072

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Y. Tanaka, S. Okuda and T. Takahashi1*UDGXDWH 6FKRRORI (QJLQHHULQJ 2VDND 3UHIHFWXUH 8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  The coherent transition radiation
(CTR) from electron bunches of a linear accelerator (linac) has continuous spectra from a submillimeter to millimeter wavelength range corresponding to the terahertz(THz) frequency range. It is a picosecond pulsed lightand hence, has extremely high peak-intensities comparedwith the other THz light sources. The light source systemusing the CTR from the electron beams of the 45 MeV
L-band electron linac was established at Kyoto University
Research Reactor Institute (KURRI) [1-3]. This CTR
light source developed has been applied to absorption
spectroscopy. Recently, the possibility of any nonlinear
effects was found in the measurement of the absorption
spectroscopy at KURRI.
However, biological effects of the radiation are unclear.
The main purpose of the present work is the investigationof the biological effects of the high-intensity pulsed CTR
using a gene of fruit fly, 'URVRSKLODPHODQRJDVWHU
(;3(5,0(17$/ 0(7+2' The electron linac at
KURRI was used in the experiments. In most experiments the beam energy, macropulse length and the repetition rate are 42 MeV, 47 ns and 60 Hz, respectively. The
experimental configurations for the absorption spectroscopy are schematically described in our previous report[4] and the details of the methods for the measurements
are described in ref. 2 and 3.
The detection method of effect on the stability of thegene was performed using the PZK (PXOWLSOH ZLQJ KDLU)
gene of 'URVRSKLODPHODQRJDVWHUas described in ref. 5 If
the CTR have any effect on the gene, the mutation frequency rate will increase or decrease. The frequency is
calculated as the small spot or large spot rates. The irradiation experiment was performed by packing the larvae
in a container with glass, plastic cylinder and sponge,
then the larvae were put in the path of the CTR, while thenon-irradiated control larvae were put near the irradiatedsample outside the path. Duration of irradiation was 2, 4
and 6 hrs. After irradiation the larvae were transferred
into new culture vials.

5(68/76$1'',6&866,21
As shown in Fig.1, by irradiation of CTR for 2 and 4
hours, the small spot rate apparently increased comparedwith the non-irradiated control groups, while the large
spot rate decreased compared with the non-irradiatedcontrol groups, however, this phenomenon seems to bewithin the variation because the large spot number wasvery scarce. By irradiation of CTR for 6 hours, both ofsmall spot rate and large spot rate were similar with the
non-irradiated control groups. Thus, irradiation of CTR
for 2 and 4 hours could cause mutation or deletion of thewild-type PZK gene, or chromosomal disjunction.

Fig. 1 Change of spot frequency by CTR (Teraherts
wavelength). Spot frequency was calculated by small oflarge spot No./wing No.
5()(5(1&(6>@ T. Takahashi et al., Rev. Sci. Instrum.  (1998) 3770.
>@ S. Okuda and T. Takahashi, Infrared Phys. Technol. (2008) 410.
>@ S. Okuda and T. Takahashi, J. Jpn. Soc. Infrared
Science & Technology 25 (2016) 49 (in Japanese).
>@ S. Okuda Y.Tanaka and T. Takahashi, KUR Progress
Report 2018, (2019) CO6-17
>@ Y.Tanaka et al., Eastern Medicine, 28 (2012) 21-35.

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&2
6WUXFWXUDO DQDO\VLV RI PXOWLGRPDLQ SURWHLQ DV VWXGLHG E\ FRPSOHPHQWDU\ XVH RI
PROHFXODUG\QDPLFVVLPOXODWLRQDQGVPDOODQJOH;UD\VFDWWHULQJ
R. Inoue, A. Okuda, M. Shimizu, K. Morishima, N. Sato,
R. Urade, and M. Sugiyama,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Under physiological condition, it is well recognizedthat most of proteins including multi-domain proteins are
not fixed to certain configurations but rather dynamicallyfluctuating due to their internal dynamics [1]. The internal dynamics of protein are considered to be deeply related to the development of their functions, hence characterization of internal dynamics such as time constantand spatial scales are essential for revealing the mechanism of their intrinsic functions. The advantage ofsmall-angle X-ray scattering (SAXS) measurement is thatit can study the structure of protein under near physiological condition: solution state, hence the possible dynamics in it is essentially observable from this technique.
Recently, molecular dynamics simulation (MD simulation) enables to identify the internal dynamics of protein.
Therefore, the complementary use of SAXS and MD
simulation would offer the better opportunity for identifying the possible internal dynamics of protein. As a firststep of work, we firstly performed structural analysis offour-domain protein through the complementary use of
SAXS and MD simulation.
(;3(5,0(176The preparation and purification of four-domain protein should be referred to our future paper [2]. SAXS
measurement was performed with NANOPIX (Rigaku
Corporation, Japan). X-rays from a high-brilliance
point-focused X-ray generator (MicroMAX-007HF, Rigaku, Tokyo, Japan) were focused with a confocal mirror(OptiSAXS) and collimated with a confocal multilayer
mirror and two pinholes collimation system with thelower parasitic scattering, “ClearPinhole”. The scattered
X-rays were detected with a two-dimensional semiconductor detector (HyPix-6000, Rigaku, Tokyo, Japan). The
sample-to-detector distance and wavelength of X-ray
used for present work was 1320 mm and 1.542 Å, respectively. For removal of unfavorable aggregates from thesample solution, the laboratory-based SEC-SAXS System(LA-SSS) was employed to measure the SAXS profile inthe 4 range (0.01 Å-1–0.2Å-1) [3]. As for MD simulation,
we performed both all-atom and coarse-grained MD
simulation. All the measurement and calculations were
performed at 25 ºC.
5(68/76 Figure 1 shows the SAXS of four-domain
protein. Firstly, we compared the SAXS profile calculated from the snapshot of All-atom MD simulation to experimentally observed SAXS profile. The calculated
SAXS profile could not reproduce the SAXS profile

Fig. 1. SAXS profile of four-domain protein (circle).
The dotted and continuous lines correspond to thecalculated SAXS profile from the snapshot fromall-atom MD and CG MD simulation, respectively.
adequately. We also calculated the SAXS profiles form
several snapshots from all-atom MD simulation, however
all the extracted snapshots could not reproduce the SAXS
profile especially at the 4 region lower than 0.10 Å-1. It is
expected that present all-atom MD simulation could not
sample the possible configurations of four-domain protein within MD simulation time. Performing the longer
time all-atom MD simulation is one of the solutions for
improving the sample efficiency, however it will also
increase the computational cost as well. In order to overcome such situation, we also performed coarse-grained
MD (CG-MD) simulation. The advantage of CG-MD
simulation is the increase of sampling efficiency due tocoarse-graining an amino acid residue as a sphere. A
snapshot was extracted from the trajectory of CG-MD
simulation and the corresponding SAXS was calculated
based on it. The calculated SAXS profile from CG-MD
simulation is also included in Fig. 1. Compared to theresult of calculation with all-atom MD simulation, the
CG-MD derived SAXS profile could reproduce the
SAXS results nicely, implying the high sampling efficiency with CG-MD calculation.
At present, we are trying to analyze the trajectory from
CG-MD calculation to figure out the internal dynamics ofthis four-domain protein. It is expected that the complementary use of MD simulation and SAXS measurements
will contribute to identify the functionally relevant internal dynamics of multi-domain protein.
5()(5(1&(6[1] J. A. McCammon, and S. C. Harvey , Dynamics ofProteins and Nucleic Acids., (Cambridge University
Press, 1987).
[2] A. Okuda HWDO., LQSUHSDUDWLRQ
[3] R. Inoue HWDO., 6FL5HS  12610 (2019).

31082

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2OLJRPHULFVWUXFWXUHDQGLWVWHPSHUDWXUHGHSHQGHQWFKDQJHRI
+VS%IURP&KLQHVHKDPVWHURYDU\FHOOM. Yohda, M. Nakamura, K. Morishima1, R. Inoue1,
M.Sugiyama1'HSDUWPHQWRI%LRWHFKQRORJ\DQG/LIH6FLHQFH7RN\R
8QLYHUVLW\RI$JULFXOWXUHDQG7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21Small heat shock protein (sHsp) is aubiquitous molecular chaperone with a relatively small
molecular weight. The characteristic feature of sHsp is the
α-crystallin domain, which is named after the α-crystallinin vertebrate lenses. Among mammalian sHsps, HspB1,
also known as Hsp27, is the most ubiquitous one. Previously, we reported the structure and function of HspB1
from Chinese hamster (&ULFHWXOXV JULVHXV) ovary cells(CgHspB1). SEC-MALS and SAXS analyses suggested
the 16mer structure of CgHspB1 [1]. However, there exist
several contradicting reports on the oligomeric structuresof HspB1[2, 3]. HspB1 may take various oligomeric conformations. In this study, we analyzed the oligomeric
structure of CgHspB1 by analytical ultracentrifuge (AUC).
In addition, we examined the effect of the deletion of the
C-terminal region and the N-terminal region.
(;3(5,0(176 CgHspB1 variants (WT, Wild type;
S15D, phosphorylation mimic mutant; DelN, N-terminal
deletion mutant; DelC, C-terminal deletion mutant) wereexpressed in (FROLand purified by anion exchange chromatography and size-exclusion chromatography. To suppress nonspecific hydrophobic interaction, size exclusion
chromatography was carried out using a buffer containing
20% ethylene glycol. The oligomeric conformation of
CgHspB1 variants were investigated by size exclusion
chromatography on HPLC (SEC), electron microscopy,
and analytical ultracentrifugation (AUC).
5(68/76 We speculated that the previous observations of various oligomeric conformations should be dueto the nonspecific interaction by the hydrophobic surface
of sHsp. Thus, we purified CgHspB1 variants by gel filtration chromatography using the buffer containing 20% ethylene glycol (Fig. 1). The purified WT and S15D exist as
large oligomers and dissociate to small oligomers at theelevated temperature in SEC. DelN appeared as small oligomers without any temperature-dependent change. Curiously, DelN was digested into two fragments by protease.
DelC appeared as various conformations. Then, WT and
S15D were examined by AUC using a buffer containing
20% ethylene glycol. At 4°C, WT appeared as a single
peak of 18mer (Fig. 2). The sedimentation coefficient increased as the elevation of temperature. At 40°C, it seemed
to form 30mer. The conformation change is reversible. Itchanged to the original conformation by lowering the temperature. In addition, small oligomers of about 6mer and12mer were also observed. Almost the same results wereobserved in S15D.

Based on these observations, we propose the following
conformational change model. The structural unit ofCgHspB1 is 6mer. In the inactivated condition, it assembles to 18mer. At the elevated temperature, they dissociate
and reassemble to the activated conformations of 24mer or
30mer. They return to 18mer by lowering the temperatures.
The N-terminal region is responsible for the assembly of 6
mers, and the role of the C-terminal region is the stabilization of oligomeric structures. 

Fig.1 SEC analyses of CgHspB1 variants
Fig. 1.

Fig. 2 AUC analyses of CgHspB1 WT

5()(5(1&(6[1] E. Sha HWDO, FEBS Open Bio.,  (2019) 1826-1834.
[2] J. Behlke HWDO, FEBS Lett.,  (1991) 119-122.
[3] B. Lelj-Garolla HWDO, J. Mol. Biol.,  (2005)
631-642.

31083

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K. Ono1, T. Aihara1, H. Tanaka2, Y. Tamari㸰, T.
Watanabe2, S. Suzuki2, S. Masunaga2
.DQVDL%1&70HGLFDO&HQWHU2VDND0HGLFDO&ROOHJH,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\

,1752'8&7,21  Tumor tissue consists of tumor
cells and stroma, especially the vasculature that supplies
the cells with oxygen and nutrients. The antitumor effectin BNCT is almost specific to cells accumulating boron
compounds. In this study, we compare the effect of thistumor cell-specific BNCT with the effect of X-rays thathas no tumor cell specificity, and quantitatively elucidate
the effect of damage caused in the vascular system on theoverall antitumor effect. This is the purpose of this research.
In fiscal 2019, prior to research on tumors, we conducted
an experiment to confirm the effect of BNCR on normal
tissue cells.This article reports the experimental results.
(;3(5,0(176 Mice and Irradiation of X-rays or
neutron. 8-week-old C3H/He mice were prepared. The
abdomen was irradiated with 10 Gy of photons 12 hours
prior to the BPA-neutron irradiation. The rest of the abdomen was shielded with a lead plate. Two and half hours
before neutron irradiation, 10B-BPA in the form of a fructose complex (300 mg/kg body weight in terms of BPA)
was subcutaneously administered to the mouse. The
blood boron concentration at the time of irradiation was
15.2 ppm. The irradiation dose to the mouse was changed
by changing the distance from the neutron beam exit holein four steps, so that a single irradiation (30 minutes)
gave four different doses. The control group of neutron
irradiation alone was similarly irradiated. The highest
neutron flux was 1.88x109/cm2s. The flux was determined by the amount of activity induced in the gold foil.
Evaluation of radiation responsiveness using regeneration of intestinal crypt cells. Three and half days after
neutron irradiation, a 10 cm long intestine was excisedfrom the same predetermined site in the jejunum, and 3
specimens were cut out. After fixing with 10% formalin,
histopathology microslide with HE staining was prepared,
and the number of crypts in which regeneration was observed on the inner circumference of the intestinal wall
was counted under a microscope.
Radiation sensitivity analysis. The relationship between
the number of crypts in which regeneration was recognized and the neutron fluence was plotted in a semilogarithmic plot, and the slopes of the curves of the neutron
alone group and the BPA-neutron group were compared.
Since the doses of neutrons themselves and the amount of
gamma rays accompanying them are equal at the same
irradiation position, the difference in the slope is derived

from the neutron reaction with BPA boron. The neutron
fluenceI0 similar to the dose D0 was obtained, and thedifference in I0 was converted into the dose due to thereaction of BPA boron and neutrons, and the D0 at theboron-neutron reaction dose of BPA was obtained. Here,it was assumed that the concentration of boron in thecrypt cells was equal to the concentration of boron inblood.
5(68/76DQG',6&866,21The results are shown in
the figure. As can be seen in the figure, the I0 of the
BPA-neutron irradiation group (closed circle), that is, theneutron fluence required to reduce the number of crypts
by e-1, is 0.925x1012/cm2. The D0 calculated from thisfluence value and the boron concentration of 15.2 ppm
was 1.04 Gy. Data on such intestinal crypt susceptibility
have not been reported yet, but are unexpectedly large.
Incidentally, the D0 of gamma rays is about 1.3 Gy. It isvery interesting to see how the values obtained this timeagree with the estimated value by N/C ratio of the cell(Ono's equation). However, this requires to know boron
concentration in the crypt cell, and it is a future research
topic. I believe that the high-SUHFLVLRQĮ-autoradiography
developed by Ono and Tanaka will be useful for that
purpose.

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WKH5DGLRORJLVWWKHGE\/,33,1&277:,//,$06 :,/.,16D:2/7(56./8:(5>@ .2QRHWDO-RXUQDORI5DGLDWLRQ5HVHDUFK
9RO1RSS±
>@ .2QRHWDO$SSOLHG5DGLDWLRQDQG,VRWRSH
9RO

31095

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2EVHUYDWLRQ RI :DWHU 8SWDNH LQ $OWHUQDWH *UDIWLQJ RI
7RPDWR DQG (JJSODQW XVLQJ '2 DV 7UDFHU


1 I
ln
x
I
The distance of neutron transmission x is equal toplant shoot diameter in this case. The initial neutron
intensity I and that of at the certain time pointI  are pixel value of those of the neutron images,
respectively.
As a region of interest (ROI), we observed changes
in the neutron attenuation coeﬃcient with a plantshoot length of 5 mm near the roots. However,Plant transpiration indicated by D2 O uptake is highlyinﬂuenced by plant size. Therefore, the changes in theneutron attenuation coeﬃcient were compared by per
dry mass (Mdry ) of the samples. Figure 1 shows thehistory of the amount of the change in the neutron
attenuation coeﬃcient, (μ − μ )/Mdry . Signiﬁcanceμ − μ =

8 0DWVXVKLPDɼ1.XERWDɼ',WR < 6DLWR  DQG +
6KRQR)DFXOW\ RI $JULFXOWXUH ,ZDWH 8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU
6FLHQFH .\RWR 8QLYHUVLW\


0.6
0.4

  ' /Mdry (mm

0.0
0.6
0.4
0.2
0.0
0.6

Without grafts

RESULTS:TheneutroncrosssectionofD2Oismuch
lower than that of water. On another note, chemical
characteristics of D2O is similar to water. Therefore,
plantcanuptakeD2Othroughtherootsystem.Inthepresence of D2O, neutron attenuation ﬁrst decreased
from the shoot part near the roots then toward theupper shoot part. The plant neutron image becamebrighter by increasing the D2O content in it.
Therefore,increasingtheD2Ocontentinplantshootscan cause changes in neutron attenuation, which canbe calculating by neutron imaging. The amount ofchange in the neutron attenuation coeﬃcient iscalculated as the diﬀerence in initial attenuationcoeﬃcient(μ)andthatofatacertaintimepoint(μ).
Changes in the neutron transmission coeﬃcient iscalculatedusingfollowingequation:

1

)

0.2

The same plants

MATERIALSandMETHODS:4kindsofgraftedsamples, including tomato grafted onto eggplantrootstock (T/E) and tomato rootstock (T/T), andeggplant grafted onto tomato rootstock (E/T) andeggplantrootstock(E/E)wereprepared.Tomato(TO)and eggplant (EO) without grafts were prepared ascontrol plants. The tomato and eggplant seedlings
weregraftedonthe23thofAugust2019,after29and30 days from sowing, respectively. Control samples
wereselectedfromtheseedlingsthatweresownatthesametimewithseedlingsforgraftedplants.Fourdays
aftergrafting,thesamplesweretransplantedintoglass
tubes ﬁlled with glass beads in order to deliver quick
D2Osupply.WeperformedneutronimagingattheE2holeofKyotoUniversityReactor(KUR)fromthe3rd
to the 5th of September. After removing water fromthe glass tube using a syringe, D2O was injected intotheglasstube.Immediatelyaftertheinjection,interval
neutron imaging was started. The exposure andintervaltimeswere300sand360s,respectively.

Dierent species

INTRODUCTION:
Graft-incompatibility
isknown to increase hydraulic resistance at the graftedjoint. Large hydraulic resistance at the grafted jointdue to graft-incompatibility is expected to produce
sweet tomato fruits by limiting water uptake.
However, Such graft-incompatibility may cause
plant death [1]. It is important to know how muchwater uptake can be limited by graft-incompatibility.
We observed water uptake in alternate grafting oftomato and eggplant by using neutron imaging anddeuterium oxide (D2O) as tracer.

0.4
0.2
0.0
10

20

30

40

50

Treatment
E/E
E/T
EO
T/E
T/T
TO

60

Time (min)Fig. 1. History of the amount of change in theneutron attenuation coeﬃcient, (μ−μ )/Mdry . Rows
in matrix of the graphs were divided by 3 groups,
namely grafted with diﬀerent spices, grafted with thesame plants, and without grafts.
tests were performed using the Tukey HSD test (n=3). There was no signiﬁcant diﬀerence between thesix groups. The tomato and eggplant without grafts
showed the same changes in neutron attenuation.
The uptake of D2 O might be similar among tomatoand eggplant when without grafts. On anothernote, samples that were grafted with the same plants
variedlychanged. Itmeansthatthewoundsproducedby grafting strongly inﬂuenced sample growth forthose that were grafted with the same plants (T/Tand E/E). Interestingly, the eggplant grafted on thetomato rootstock (E/T) showed the second highest
change in neutron attenuation. In previous studies,
eggplantgraftedontomatorootstockproducedlarger
roots [1]. The large tomato roots of the E/T sample
supposedly contributedto the increased D2 O uptake.
REFERENCES:[1] M. Oda et al., J. Japan. Soc. Hort. Sci., 74(6),458-463 (2005)


‑217‑

&2

3URGXFWLRQRIPHGLFDOUDGLRLVRWRSHVXVLQJHOHFWURQOLQHDUDFFHOHUDWRU

S. Sekimoto, T. Ohtsuki

5(68/76 The results of the TcMM applied to the
MoO3 pellets irradiated with bremsstrahlung photons
are shown in Table 1. The activities of 99Mo and 99mTc in
the natMoO3 solution prepared in the first step of the
TcMM and the solution obtained from the final step ofTcMM, and the chemical yield of 99mTc are presented inTable 1. The table header ‘Run No.’ 10-1 and 15-1 indicate the results for the solutions containing dissolved natMoO3 pellets irradiated with bremsstrahlung photons of(e’s of 25 and 30 MeV, respectively. In contrast, ‘Run
No.’ 10-2 and 15-2 are the results for the solution wheretransient equilibrium has been reached between 99Mo and99m
Tc after the initial milking of 99mTc in the 10-1 and15-1 solutions. The chemical yield of 99mTc ranged between 83 to 99% over the four runs of the TcMM. In particular, the activity of 99Mo in the solution collected by
the TcMM was low, being below the detection limit of J-ray spectrometry. This can also be confirmed by examining the J-ray spectra of the natMoO3 solution before the
TcMM and the solution collected by the TcMM. Those
spectra were reported in ref. [8].
nat

,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  A shortage in the supply of 99Mo
resulting from the shutdown of reactors used for its production is a global problem. Because 99Mo is an indispensable source of 99mTc, which is used in nuclear medicine to make diagnoses using techniques such as scintigraphy and single photon emission computed tomography(SPECT), a stable supply of 99Mo is vital. Therefore,
production of 99Mo by using neutrons or protons generated in accelerators has been investigated [1–3]. To separate 99mTc from 99Mo produced by an accelerator, methods based on sublimation, solvent extraction, andion-exchange column chromatography have been examined and developed [2,4–6]. In addition, Gopalakrishna et
al. have reported the preparation of 99Mo by the
100
Mo(J,n) reaction using bremsstrahlung photons [6],followed by conventional solvent extraction using methyl
ethyl ketone (MEK) and zirconium (Zr) molybdate gel toseparate 99mTc. According to the regulations of the Japanese pharmacopeia, the extraction using organic materials
and the gel method using heavy metal elements such as
Zr are not approved for the 99mTc-separation methods.
Additionally, it is also difficult and impractical to use thesublimation method, which requires complicated and/or
large scale devices for the mass-production of pure 99mTc.
Recently, Kaken Inc. developed a new method, known as
the “technetium master milker” (TcMM). This technique
can produce highly pure 99mTc at a maximum activity of
1.85 × 1013 Bq (500 Ci) per batch from 99Mo of low specific activity [7]. We carried out the production of 99Mo
by the 100Mo(J,n) reaction using bremsstrahlung photons
generated in an electron linear accelerator (LINAC), atechnique that has not been investigated significantly inJapan. The amounts of 99Mo produced at several electronenergies ((e) were examined. To separate 99mTc from theirradiated target, in this work, the TcMM was applied tothe 99Mo produced by LINAC, and the subsequent yieldof 99mTc was evaluated.

5()(5(1&(6>@ Y. NagaiHWDO, J. Phys. Soc. Jpn.,  (2013) 064201
>@ Y. Nagai HWDO, J. Phys. Soc. Jpn.,  (2014) 08320
>@ K. Nakai HW DO, Proc. Jpn. Acad. Ser. %  (2014)
413–421.

>@ M. Kawabata HW DO, J. Phys. Soc. Jpn.,  (2015)
023201
>@ K. Mang’era HW DO, J. Radioanal. Nucl. Chem., (2015) 79-85.
>@ A. Gopalakrishna HW DO, J. Radioanal. Nucl. Chem., (2016) 431-438.
>@ K. TatenumaHWDO, Radioisotopes  (2014) 501-513.
>@ S. Sekimoto et al., J. Radioanal. Nucl. Chem., (2017) 1361-1366.

(;3(5,0(76  The TcMM applied to the irradiatednatMoO3 pellets was essentially the same as that reported
by Tatenuma et al. [7]Table 1Yield of 99mTc from bremsstrahlung photon-irradiated natMoO3 by TcMM process
(a Second crop, b End of bombardment, c Detection limit)

Run
No.

Weight of natMoO3 & (e

10-1
10-2a
15-1
15-2a

0.97 g,25 MeV
0.96 g,30 MeV

Elapsed timefrom EOBb
(h)
213.2
237.3
215.3
239.2

Activity in natMoO3 solution (Bq)
99
99m
Mo
Tc
4.91E+04
5.40E+04
3.74E+04
3.98E+04
1.15E+05
1.26E+05
5.20E+04
8.48E+04

31131

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Activity in solution collectedby TcMM process (Bq)
99
99m
Mo
Tc
c
<DL
5.05E+04<DLc
3.33E+04<DLc
1.19E+05<DLc
8.33E+04

Yield of
Tc
(%)
93.5
83.7
94.2
98.3

99m

&2

N-Acetylneuraminic acid functioned as the scavenger for reacive oxygen species
generated by the gamma-ray irradiation

N. Fujii1, S. Kishimoto1 and T. Takata2
12Radioisotope Research Center, Teikyo University
Institute for Integrated Radiation and Nuclear Science,
Kyoto University

INTRODUCTION:
N-Acetylneuraminic acid (Neu5Ac) is a sialic acid,
which occurs in mammals, certain mollusks, and somemicroorganisms, and is found a capping suger in the oligosaccharide chains of glycoproteins and glycolipids [1].
Most studies on glycanic Neu5Ac have focused primarilyon cell protection, fertilization, immunology, inflammation and tumors [2-4]. Free Neu5Ac molecules is oxidized by H2O2 to provide its decaroxy product,
4-(acetylamino)-2,4-dideoxy-D-glycero-D-galacto-octonic
acid (ADOA) [5]. Therefore, monomeric Neu5Ac is thepotent defense molecule against oxidative damage.
Ionizing radiation decomposes water and generates
free radicals and reactive oxygen species. Then we expected the monomeric Neu5Ac might be scavenged thereactive oxygen species generated the ionizing radiation.
In this study, we developed the method to quantitate thepotential scavenging reaction of Neu5Ac for gamma-ray
irradiation. In order to test our methods, we irradiated
Neu5Ac solution with gamma-ray, then quantitatedproduct (ADOA) by liquid chromatography–tandem mass
spectrometry (LC-MS/MS) using by our developed
method.
EXPERIMENTS:
Material Nu5Ac was dissolved in water, and the pH of
the solution was adjusted to 7.0 with sodium hydroxide.
Gamma-irradiation Gamma-irradiation was carried out
at the Co-60 Gamma-ray Irradiation Facility of the Kyoto
University Institute for Integrated Radiation and Nuclear
Science. Nu5Ac aqueous solution were irradiated withgamma ray at a dose rate of 943 Gy/h.
Quantitation of ADOA The quantitative analysis of
ADOA was used by LC-MS/MS. The high performanceliquid chromatography was used a U3000HPLC system(Thermo Fisher scientific). The column was CAPCELL
CORE PC (OSAKA SODA, 2.7 μm, 2.1 mm I.D.×100mm). A sample were eluted with a flow rate of 0.2
mL/min and an isocratic mode with mobile phase (75%acetonitrile, 25% water, 10 mM ammonium formate, pH
3.5). The mass spectrometer was used Q Exactive(Thermo Fisher scientific). ADOA was measured by parallel reaction monitoring (PRM) in the positive ion mode,using transitions m/z 282.11 → m/z 186.07

PRM method was set the optimal for commercial standard. Then, the method was used for Neu5Ac aqueous
solution aftergamma-ray irradiation.

Fig. 1. Production of ADOA from Neu5Ac by irradiation with gamma-ray
Fig. 1 show the production of ADOA from 100mM
Neu5Ac aqueous solution irradiated with gamma-ray atdoses of 0, 0.5, 1, 3 and 5 kGy. As the radiation dose wasincreased, the production of ADOA increased. The 1 kGy
gamma-ray irradiation for 100 mM Neu5Ac solution increased the ADOA amount to 184 μM (Fig. 1), suggested
the yields of ADOA from Nu5Ac was 0.184 %. On theother hand, in 10 mM Neu5Ac solution, the yields of
ADOA from 1kGy gamma-ray irradiation was 1.34 %(data not shown). The lower concentration of substrate,
the higher yields of ADOA, suggested that gamma-ray
promotes reaction from Neu5Ac to ADOA via formationof reactive oxygen species (H2O2) in solvent (indirect
action).
Those results suggested monomeric Neu5Ac as scavenger for reactive oxygen species generated by the gamma-ray irradiation.
REFERENCES:[1] R. Schauer R., Zoology, 107 (2004) 49-64[2] T. Angata et al., Chem. Rev. 102 (2002) 439-469[3] R. P. Crocker, Curr. Opin. Struct. Biol. 12 (2002)
609-615[4] K. Takayama et al., Proc. Natl. Acad. Sci. USA 93(1996) 10662-10667[5] R. Iijima et al., FEBS Lett. 561 (2004) 163-166

RESULTS:To quantitatively investigate the amount of ADOA,

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&2 Preliminary analysis of structural composition of menaquinone-7 produced by
Bacillus subtilis natto
to-MK-7, of which molecular weight was presumed to be

T. Chatake, Y. Yanagiswa1, A. Okuda, K. Morishima, R.
Inoue, M. Sugiyama,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
1Faculty of Pharmaceutical Science, Chiba Institute of
Science
INTRODUCTION: Natto is a Japanese traditional
fermented food, which is made of soybeans. It attracts agreat attention from the point of view of nutrition, because it contains various kinds of physiologically active
substances. In particular, menaquinone-7, which is a kindof vitamin K2, is abundantly contained in natto [1]. In
Japan, young women intake 99% of menaquinone-7

80~100 kDa, was not observed. A peak with m/z = 656
corresponds to menaquinone-7㻌 (MW~650). Most significant peaks were around m/z = 1050, implying that
KBF is smaller than 3kDa, of which value was estimate by SDS-PAGE. In addition, the plural number ofthe peaks suggests the variation of the amino acid sequences of KBF.
It is just the first data of mass spectroscopy of natto-MK-7. The further experiments are under planning.

from pulses including natto, and the pulse food is themain source of vitamin K (45.1%) for the natto eaterof the young Japanese women [2]. Menaquinone-7
produced by Bacillus subtilis natto (natto-MK-7) has aremarkable physiochemical property. All types of vitamin K are water-insoluble compounds. Meanwhile,
natto-MK-7 is a water-soluble macromolecular complex, of which molecular weight is estimated to be
80~100 kDa by size-exclusion chromatography [3,4].
This property has an advantage on application offood/medical uses: pharmaceutical preparation, supplements, and food manufacture. Previously, Ikeda andDoi reported that the complex is composed of ~3kDa
glycopeptides named K-binding factor (KBF) [3]. Our
recent study of highly purified natto-MK-7 indicatedan additional component with the molecular weight of~11 kDa [5]. However, the detail information about thestructural components of natto-MK7 is still unknown.
In the present study, mass spectroscopy of natto-MK7
has been succeeded. Here, our new finding is shown.
EXPERIMENTS: Natto-MK-7 was produced and purified as previously reported [5]. Bacillus subtilis natto
miyagino was incubated in liquid medium containing 2%
hipolypepton-S, 3% glycerol, and 0.5% methionine. After
cultivation at 42 °C with shaking at 100 rpm for 7 days,
liquid medium was concentrated before purification. The
purification was carried out by fast protein liquid
chromatography. Four times of weak anion-exchange
chromatography using DEAE sepharose FF were carriedout with a gradient from 0.3 M to 1.0 M NaCl in 20 mM
Tris-HCl buffer (pH 7.6). The final step of the purification was size-exclusion chromatography using GE
HiPrep 16/60 Sephacryl S-300HR in 20 mM Tris-HCl
buffer (pH 7.6) and 0.1 M NaCl. Mass spectroscopy wasmeasured by MALDI-TOF/MS (microflexLT).
RESULTS: As shown in Fig. 1, mass spectra of natto-MK-7 could be observed for the first time. Strong
peaks with m/z < 600 are derived from the matrix used
for TOF/MS. Significant peaks could not be observed at
m/z > 10,000, indicating that the whole structure of nat-Fig. 1. The results of mass spectroscopy of natto-MK-7 in the ranges of 0~10,000 Da (upper) and
600~1,500 Da (lower).
REFERENCES:[1] D.H. Bishop, K.P. Pandya, H.K. King, Biochem. J.
83, 606-614 (1962).
[2] M. Kamao et al., J. Nutr. Sci. Vitaminol (Tokyo) 53,
464-470 (2007).
[3] H. Ikeda, Y. Doi, Eur. J. Biochem. 192, 219-224(1990).
[4] Y. Yanagisawa, H. Sumi, J. Food Biochem. 29,
267-277 (2005).
[5] T. Chatake et al., Y. Yanagisawa, R. Inoue, M.
Sugiyama, T. Matsuo, S. Fujiwara, J. Food Biochem.
e12630(6) 1-7 (2018).

31140

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&2

Measurement of Absorption Spectra of a Humann Calcified Aorta Tissue
in the Sub-Terahertz Region, which Dependented on the Thickness (III)N. Miyoshi and T. Takahashi1

spot type (CL-P030, Keyence, Osaka, Japan).

Department of Molecular Chemistry, Kyoto Institute ofTechnology
1Institute for Integrated Radiation and Nuclear Science,
Kyoto University

RESULTS and DISCUTION: (1) The thickness ofsamples on the three points were measured as shown inf
Fig. 2. A (calcified deposition) =0.0929, B (cholesterol
deposition) =0.837, C (protein deposition) =0.379 mm,
respectively.

INTRODUCTION: The LINAC (Electron linear accelerator) technology in the millimeter- and terahertzwaves had been unique and had been used as a coherent
synchrotron light source in the Institute for Integrated
Radiation and Nuclear Science of Kyoto university(KURNS) to observe the transmittance spectra of a human calcified aorta tissue as a collaborate study. The absorption spectra in the sub-terahertz region had been not
so clear for the raw tumor tissue although Ashworth-PC.
et al. [1] had reported for the excised human breast cancer by a terahertz pulsed spectroscopy observed at 320
GHz, which was estimated a longer relaxation timecomponent of the induced electricity for water molecules[2-3] in the raw tumor tissue for three years at the linear
analysis.
We had started to measure of new biological sample of a
calcified human aorta dried tissue sampling from thepathological autopsy in the last year. Furthermore, thegetting spectral information was estimated with the
SEM-EDX elements images of the calcified aorta tissue
with a biological meaning in this year. It was reported therelation of the biological information between both of theelement images and sub-THz spectral components in thisreport.
EXPERIMENTS: (1) Instrument of Near-field in Terahertz Region: The photograph of the instrument was
shown in Fig. 1. Mark-A: Pre-probe Wiston cone;50-10mm diameter, Length=60mm; the irradiate diameter=0.775mm; Mark-B: The concentrate light probe (diameter=3mm). The instrument was developed by Dr. T.
Takahashi [4] for the transmittance measurements.

A

B

Fig. 1. The near field area of sample holder position.
(2) Measurement of the Thickness of Sample: .
The thickness on the three points was measured by a laser

A

C

Fig. 2. The absorption spectra at 3 points (A: calcified
point), the (B: cholesterol deposition, C: protein
deposition) of a human aorta blood vessel wall,
respectively.
(2) The absorption spectra of the sample tissue for eachpoints A, B and C were measured according the different
thickness points as shown in Fig. 2, which might bechanging the refraction to dependent on the thickness
values. It was different from the last reported spectra alittle.
In the results, the absorbance of the dried tissue at 248
and 522 GHz were observed in the calcified area (included of CaPO4 components from the data of SEM-EDX
analysis of calcified aorta tissue), and the absorption
peaks of 330, 620 GHz were observed in the cholesteroladhesion area. In the both areas, it was observed the absorption peaks at 500 and 659 GHz also.
In this report, it can report of more detail analysis
combined with the thickness information data of the dried
tissue by an laser measurement technology.
REFERENCES:>@ Phillip C. Ashuworth et al., Optics Express, 17 (2009)
12444-12454.
>@ Toshiko Fukasawa, et al., Phys. Rev. Lett., 95 (2005)
197802.
>@ Hiroyuki Yada, et al., Chem. Phys. Lett., 464 (2007)
166-170.
>@ T. Takahashi, et al., J. Phys.: Conf. Ser. 359 (2012)
012016-1-4

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%RURQQLWULGH %1 DSURVSHFWLYHPDWHULDOIRUERURQQHXWURQFDSWXUHWKHUDS\Manjo Kaur1, Paviter Singh, Kulwinder Singh, Usha
Singh Gaharwar, Ramovatar Meena2, Manjeet Kumar,
Fumiko Nakagawa, Shangze Wu, Minoru Suzuki, Hiroyuki Nakamura, Akshay Kumar$GYDQFHG)XQFWLRQDO0DWHULDOV/DERUDWRU\'HSDUWPHQW
RI1DQRWHFKQRORJ\6UL*XUX*UDQWK6DKLE:RUOG8QLYHUVLW\3XQMDE,QGLDBNCT study of 10BN was studied in comparison to L-BPA.
Fig. 1(a) shows the schematic representation of 96-wellplate irradiation. HeLa cells treated with 10BN shows almost similar dose-dependent cell killing effects as L-BPA
at neutron fluence range of 3.6–6.3 x 1012/cm2 (Fig.1(b)).
Thermal neutron fluence of ~6.3 x 1012/cm2 resulted in almost 50% cell death of 10BN treated cells.

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8QLYHUVLW\   &,1752'8&7,21  Boron Neutron Capture Therapy(BNCT) is an expecting cancer therapy for the treatmentof harsh and un-operatable malignant tumors. The efficiency of boron agent depends highly on tumor selectivity,
sufficient amount of boron agent in tumor site, non-toxicity, tumour/normal tissues ratio (>3) and absorption ofthermal neutrons by boron. Among a variety of bioceramics, boron nitride (BN) have remarkable properties that canbe used as investigations for diagnostic purposes and drugdelivery. In this study, 10BN was prepared using simple andcost effective solvothermal method to get the product withhighest purity. BNCT studies were performed at Kyoto
University Research Reactor Institute (KURRI).
(;3(5,0(176 Boric acid (10B enriched with 99
atom% 10B isotopic purity) and ammonia solution wereused as boron source and nitrogen respectively to synthesize 10BN by solvothermal method. Details of experimental procedure and characterization are described in theliterature.[1]5(68/76 The structure is layered with B-N layers
stacked over each other having very high surface area withelectronegative atoms which makes this material highly
dispersible in water. TEM images also shows that the particles are in 15–25 nm range interacting with each other. 
MTT assay using HeLa, MCF-7, and HEK-293 celllines was carried out. The results showed relatively
less changes with lower concentration (150 and 300 µg/mL) of 10BN nanostructures, however up to 40 percent
rate
was
observed
athighercytotoxi-city
concentration (1200 µg/mL). These results indicate thatthese nanostructures are not cytotoxic for tested cell lines
at the concentration of up to 1 mg/mL and can be used forbiomedical applica-tion at safe concentration below thestudied doses.
Intracellular boron concentration was detected and results confirm the presence of boron inside cells. Boroncontent of cells treated with 25 ppm and 100 ppm concentration was 0.57 ppm and 1.9 ppm respectively. These results indicate concentration dependent uptake of boron in
HeLa cells and ability to enter in intracellularenvironment.

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Fig. 1. (a) Schematic representation of irradiation to
96 well plate. (b) BNCT effect of 10B enriched BN
on HeLa cell lines in comparison to L-BPA.
&21&/86,21 The aim of present work was to synthesize 10B enriched nanostructured boron nitride from boric acid and ammonia solution. BN was synthesized by solvothermal method at 650 ᵒC for 24 hours. The decomposition of ammonia solution produces hydrogen which is responsible for BN formation even at relatively low temperature. BNCT studies of boron nitride were performed using thermal neutron source on HeLa cells in comparison to
L-BPA. The thermal neutron fluence of ~6.3 x 1012/cm2
resulted in almost 50% cell killing of BN treated HeLa
cells. These results show that 10B enriched BN can be used
as a potential candidate for BNCT.
5()(5(1&(6[1] A. Kumar HWDO, Materials Lett., (2020) 126832.

31017

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K. Kimura, T. Takata1, Y. Sakurai1, H. Tanaka1, and K.
Takamiya1)XMLWD&RUSRUDWLRQ,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\

5()(5(1&(6>@ K. Kimura, et al., Proceedings of 8th International Conference on Radiation Shielding, vol. 1, pp.35-42,ANS
inc, Arlington, USA, 1994.
>@ M. Kinno, et al., ANS Radiation Protection & Shielding Conference, pp.673-678, Spokane, USA, 2002.
>@ K. Kimura, et al., Proc. of Int. Conf. on Nuclear
Engineering (ICONE16), Florida, USA, May 11-15,(2008) 4848

,1752'8&7,21One of the typical materials for radiation shield is concrete at the points of its flexibility, sufficient supply, and inexpensiveness. On the other hands,
once radiation facilities with shielding concrete start to operation, the concrete are affected by the radiation ray fromthe operating radiation source in the facilities and activated.
Various types of low activation concrete[1]-[3], which are
typically white cement based concrete, are the one of theways to solve the problem. Especially, boron neutron capture therapy (BNCT) should be effective facilities to apply
the low activation concrete.
0(7+2'6 Various types of concrete samples werecrushed to certain size (typically under 0.7mm or less), andwere packed for 0.1 to 0.3 g with special treatment for theirradiation in KUR. After the irradiation with 10 to 60
minutes and with the certain cooling period, these samples
were measured by Ge detector one by one.The quantity ofthe target elements, which were selected by former invesFig. 1 Correlation of different preparations of sample
tigations as Co, Cs, Sc, Fe and Eu[1]-[3], in each sample
were estimated by the comparison of the known standard material in the same package forthe irradiation.
5(68/76 Figure 1 shows thecorrelation of the sample preparation procedures (typical andadditional with disc mill) for
measured contents of elements
and introduces each result by
two preparation methods issimilar. Metal disc mill wasused for crushing the samples
additional to typical proceduresamples, in order to reduce theFig. 2 Distribution of Eu and Co in various concrete
grain size down to a few tenthmicrometer. Figures 2 and 3
show the distribution of Eu, Co,
and Cs contents in while cement based concrete (39 samples) and ordinally concrete (52samples).
&21&/86,21 More than
200 concrete samples were prepared for estimating the contents of Eu, Co, and Cs, including investigation of preparationof the samples. These data
would contribute the establishment of material data forshielding materials.
Fig. 3 Distribution of Cs and Co in various concrete

31021

‑224‑

&2(YDOXDWLRQRIWKHDEVFRSDOHIIHFWREVHUYHGE\PRXVHKHDG
LUUDGLDWLRQIROORZLQJWKHUPDOQHXWURQLUUDGLDWLRQ

Y. KinashiDQG T.Takata,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\,1752'8&7,21 The effect of metastasis of lymph
nodes such as lymph nodes in areas that are not irradiatedsites in radiation therapy of malignant lymphoma is reported in 1953 and is called abscopal effect. Abscopal isa Latin meaning of "far away" ab and the ancient Greek"target" scopal, a phenomenon that collectively refers to
the indirect effects of radiation on sites that are not thesites of the irradiation. It is reported about the abscopal
effect in radiotherapy that immune response is activatedby partial radiation [1]. The influence on immune organization of the mouse at the time of the head irradiation is
not well known. The purpose of this study is to evaluate
the relative biological effectiveness in the severe combined immunodeficiency (SCID), so-called SCID mice,those are having well-known high radiation sensitivity
comparing with C3H/He mice having normal radiation
sensitivity.
(;3(5,0(176
CB17/Icr-3UNGFscid/CrICrIj (SCID
mice) were obtained from Charles River Inc. As a comparison experiment for the SCID mice, C3H/He mice
were obtained from Japan Animal Inc.
Neutron irradiation was performed as follows. The
Heavy Water Facility of the Kyoto University Research
Reactor (KUR) was used. Mice were restrained in a plastic box on a radiation board. Neutron fluence was measured by radio-activation of gold foil and gamma-ray
doses by TLD. Mice were restrained in a plastic box onan acrylic plate. In order to irradiate the head of themouse, the mice head was left radially to the irradiation
area of the plate. Gold and TLD placed on the head andabdomen, respectively. The mice were fixed on tape andthe acrylic plate and mice were covered with a plastic
bag to prevent the escape. After irradiation, the spleniccell suspension was adjusted and incubated. At 48 hour,
72 hours after irradiation, apoptotic induction of the cells
was examined by Cell Death Detection ELISA (Roche).

7DEOH. Apoptotic induction of the splenocytes at 48
and 72 hours after neutron irradiation*
SCID
C3H
Radia48 h.
72 h.
48 h.
72 h.
tion
after radia- after radia- after radia- after radiadose
tion

tion

tion

tion

control

1.1 ± 0.1

1.1 ± 0.1

1.1± 0.1

1.0± 0.1

0.5Gy

1.5± 0.1

1.8± 0.2

1.1± 0.1

1.1± 0.1

1.0Gy

2.1± 0.22.5± 0.2

1.5± 0.1

1.1± 0.1*Each data shows the enrichment factor at neutronradiation dose. Each data shows the mean value ±SD.
',66&866,21
Previously we reported the RBE values for SCID miceof the LD50 by radiation oral death assay and gamma
H2AX foci number of the lymphocytes. The RBE
values calculated from radiation oral death assay andgamma H2AX foci number of the lymphocytes were
1.6 for SCID mice and 2.0 for C3H mice [2]. The.
SCID mice show extreme sensitivity to ionizing radiation, because cells lack functional DNA-dependent
protein kinase. In this study, our results suggest thatthe abscopal effect for SCID mice were larger thanC3H mice. The difference of the apoptosis of thesplenic cells between SCID mice and C3H mice waslarger on the time dependent. That is to say, the hyper radiation sensitivity was observed in the abscopal
effect after the neutron irradiation.
5()(5(1&(6>@ K Reynders HW DO, Cancer Treatment Reviews,
(2015)503-510.
>@ Y Kinashi et al., ICRR 15th abstract book (2015).

5(68/76 As shown in Table 1, the apoptotic cha
radiation dose. The apoptotic induction of thespleno-cytes of SCID mice was larger than that of
C3H mice at 48 hours and 72 hours after irradiation.
The differ-ence of the apoptosis of the splenic
cells between SCID mice and C3H mice was larger
at the 72 hours than 48 hours after the neutronradiation.
BBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBBB



‑225‑

&2 7KHIHDVLEOLW\VWXG\RI(X/L&$)QHXWURQGHWHFWRUIRUDQDFFHOHUDWRUEDVHG%1&7
T. Nakamura, Y. Matsui, A. Yamaguchi, D. Nio, K. Sakasai, H. Nakashima, R. Okumura1DQG K. Takamiya1

Optical fiber-DSDQ$WRPLF(QHUJ\$JHQF\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\Thread

Plastic bottle(detector is inside),1752'8&7,21 The stability of neutron flux at anaccelerator-based BNCT facility is relatively worse thanthat at a reactor-based one. Therefore, it is necessary tomeasure the neutron flux precisely in real-time to optimize the patient’s exposure dose for the accelerator-based BNCT. However, the neutron flux is so intense(about 109(n/cm2/s)) that the real-time measurement has
not been realized yet. Hence we tried to measure the neutron flux with a small detector using a Eu:LiCAF scintillator [1] on the tip of optical fibers, as shown Fig.1. We
reported that this detector has the linearity to the neutron
flux to109(n/cm2/s) in our previous article [2]. In thisexperiment, we tried tocheck the linearity for neutron flux up to 1011(n/cm2/s)
FPusing the KUR-SLY, and to
2SWLFDOILEHU
check it can be used not(X/L&$)
only exposure dose monitor
VFQWLOODWRU
but also beam monitor.
Fig. 1 Detector coupledwith the optical fiber.

(;3(5,0(176 The experiments were performed at
the KUR-SLY where the maximum neutron flux of about1012(n/cm2/s) is available at the bottom when the reactor
power is 1MW [3]. Figure 2 shows the experimental setup for the measurement, where the photon counting unit
C8855 and 994 is able to count up to 1 Mcps. The optical
output from the Eu:LiCAF scintillator through the opticalfibers was properly converted to an electric signal andcounted with the counting units. Prior to the measurement, the detector was put into the plastic bottle, where
Figure 3 shows the situation, and loaded to 47 cm fromthe bottom of the KUR-SLY. At this position, the maximum neutron flux is about 1.81010(n/cm2/s). First experiment was carried out from the starting-up to 1
MW-arrival of the reactor. Next, after arrived at 1MW,
we changed the detector position in the KUR-SLY, tomeasure counting of different neutron fluxes using the

Fig. 3 Situation about the putting into the plastic bottle.

Fig.4 The neutron count rate with QOF
F

Fig.5 The neutron count rate wi
withith POFdetector coupled with the quartz optical fiber (QOF) or
the plastic optical fiber (POF).



5(68/76 The count rate using the detector coupledwith QOF was varied according to reactor power during
the reactor power rises to 1MW from starting-up. Figure
4, 5 show the neutron count rate using QOF and POF
respectively with the detector. The results indicate thedetector coupled with QOF or POF have approximately
linearity to the neutron flux up to 21010 (n/cm2/s).
&21&/86,216 We developed detector which is small
detector using a Eu:LiCAF scintillator on the tip of optical fibers, and confirmed that the detector coupled with
QOF has the same performance as the detector coupledwith POF. The detector can measure neutron flux of 108
to 21010 (n/cm2/s), therefore it can be used not only
exposure dose monitor but also beam monitor for accelerator-based BNCT facility.
It is confirmed that QOF is more radiation-resistant than
POF [4]. We are planning to conduct experiments to confirm the detector coupled with QOF have enough radiation-resistance for practical use in the future.
5()(5(1&(6>@ N. Kawaguchi, Doctor Thesis, Tohoku University,
http://hdl.handle.net/10097/56580>@ KURRI PROGRESS REPORT 2017 CO7-2>@ KUR-SLY http://www.rri.kyoto-u.ac.jp/JRS/>@ T. Nakamura, K. Sakasai, H. Nakashima, K. Takamiya,
H. Kumada, 2016. Characteristics of Radiation-Resistant Real-Time Neutron Monitor for Accelerator-Based BNCT.
JOURNAL OF RADIATION PROTECTION AND
RESEARCH. 41, No.2. 105-109.
DOI: https://doi.org/10.14407/jrpr.2016.41.2.105

Fig. 2 Experimental setup.

31076
‑226‑

&2 Enhancement of the cancer cell-killing effects of boron neutron capture therapy byoverexpression of LAT1 in human cancer cells
ZLWKHWKDQRODQGVWDLQHGZLWKFU\VWDOYLROHWDIWHUFHOOFXO
WXUHIRUGD\V. 2KQLVKL00LVDZD16LNDQRDQG06X]XNL
Departments of Biology, Radiological Science, IbarakiPrefectural University of Health Sciences
2
National Institute of Advanced Industrial Science and
Technology,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: 2XWFRPH IURP %1&7 ODUJHO\ GH
SHQGV RQ DPRXQW RI LQWUDFHOOXODU DFFXPXODWLRQ RI ERURQFRPSRXQG /W\SH DPLQRDFLG WUDQVSRUWHU  /$7  >@
WKURXJK ZKLFK ERURQRSKHQ\ODODQLQH %3$  LV WUDQVSRUWHG
LQWR FHOOV LV IUHTXHQWO\ H[SUHVVHG LQ YDULRXV W\SHV RI WX
PRU FHOOV LQFOXGLQJ JOLREODVWRPD EXW QRW LQ QRUPDO FHOOV>@ :H WUDQVIHFWHG pCMV/LAT1-GFP SODVPLGV LQWR D
JOLREODVWRPD FHOO OLQH 7* DQG VHOHFWHG VHYHUDO FORQHV
DQGFRQILUPHGWKDWWKRVHFORQHVVWDEO\RYHUH[SUHVV/$7
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FORQHVWKDWXSWDNH &%3$DQGWLPHVUHVSHFWLYHO\ODUJHUWKDQ7*.&FRQWUROFORQHRESULTS: 7*. FHOOV VKRZHG VOLJKWO\ HQKDQFHG
VHQVLWLYLW\ WR WKH IOXHQFHV FRPSDUHG ZLWK 7*.
7*.& DQG WKH OLSRIHFWHG 7*.& FHOOV LQ WKH
FDVHRISSP %6$WUHDWPHQW  7KHUHLVQRVLJQLILFDQWGLIIHUHQFH LQ WKH VHQVLWLYLW\ EHWZHHQ 7*. DQG7*.& FHOOV DV ZHOO DV WUDQVLHQWO\ OLSRIHFWHG
7*.& FHOOV,QWKHFDVHRISSP %6$WUHDWPHQW
7*. DQG WKH OLSRIHFWHG 7*.& FHOOV VKRZHG
ODUJHO\ HQKDQFHG VHQVLWLYLW\ WR WKH IOXHQFHV FRPSDUHGZLWK 7*.& FHOOV (5   7*. FHOOV VKRZHGVOLJKWO\HQKDQFHGVHQVLWLYLW\ (5  7KHVHQVLWLYLW\RI
WKH FHOOV WR WKH IOXHQFHV ZDV FRUUHODWHG ZLWK WKH H[SUHV
VLRQOHYHORI/$7RIWKHFHOOV)LJXUHVRIUHVXOWVDUHQRZ
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CONCLUSION: 7KLVVWXG\VKRZHGWKDWRYHUH[SUHVVLRQ
RI /$7 LQ FDQFHU FHOOV FDXVHV HQKDQFHG DQWLFDQFHU HI
IHFWVRI%1&7DQG%1&7FRPELQHGZLWKJHQHWKHUDS\LV
EHQHILFLDOIRUWXPRUVEHDULQJORZ/$7H[SUHVVLRQREFERENCES:
>@ < .DQDL et al. - %LRO &KHP 273 
>@ ..DLUDet al%U-&DQFHU107  EXPERIMENTS: 7*. 7*. 7*.& DQGWUDQVLHQWO\ pCMV/LAT1-GFPOLSRIHFWHG 7*.& FHOOVWUHDWHGZLWK/LSRIHFWDPLQHRYHUQLJKW ZHUHWUHDWHG
ZLWK PHGLXP FRQWDLQLQJ %3$   RU  SSP  IRU 
KRXUV7KHFHOOVZHUHWU\SVLQL]HGDQGWKHFHOOVXVSHQVLRQV
LQ PO FU\RWXEHV ZHUH LUUDGLDWHG ZLWK WKH IOXHQFHVRU*\LQWRWDOGRVHVRIQHXWURQVDQG UD\V IURP
.85 7KH LUUDGLDWHG FHOOV ZHUH SODWHG RQ WKUHH UHSOLFDWH
GLVKHV IRU FRORQ\ IRUPDWLRQ DVVD\ 7KH FHOOV ZHUH IL[HG



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&2&OLQLFDO2XWFRPHRI%1&7IRU$GYDQFHGRU5HFXUUHQW+HDGDQG1HFN&DQFHU

N. Kamitani1, Y. Tanaka2, Y. Fukuda3, M. Suzuki4, Y.
Sakurai4, J. Hiratsuka1
'HSDUWPHQW RI 5DGLRORJ\ 2QFRORJ\ 'HSDUWPHQW RI 'HUPDWRORJ\ 'HSDUWPHQW RI 2WRODU\QJRORJ\ .DZDVDNL 0HGLFDO
6FKRRO ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH

Number ofpatients>7DEOH@Sex

Male / Female

10 / 14

Age

Median(range)

53 (34-78) years

Histology

SCC/ Non-SCC

18 / 6.\RWR8QLYHUVLW\

Overall Survival rate
[ Fig. 1 ]0[ Fig. 2 ]

1.5

2

year

1.5year

1Overall Survival rate
[ Fig. 3 ]
0

0.5

1

1.5

2

year

Progression free survival rate

‑228‑

1

0.5

0

[ Fig. 4 ]
0



0.5

Progression free survival rate

,QWURGXFWLRQ: We report outcome of BNCT for
AHNC (advanced head and neck cancer) and RHNC
(recurrent head and neck cancer). The principal
endpoints specified in this study were progression-freeand overall survival consequences.
0HWKRGV: 24 patients (25 cases) were included in thisstudy and received BNCT between Aug. 2017 and Feb.
2019. One patient was received BNCT twice, becauseof tumor progression after first BNCT. Characteristics ofthe patients are detailed in Table1. FBPA-PET wasunder-gone in all cases to determine the indication for
BNCT, and the median T/B ratio was 3.2 (range
2.5-8). 13 pa-tients had received systemic therapy(ST), such as nivolmab, cetuximab or TS-1, and thetherapy had beencontinued for 6 months after BNCT.
Overall survival (OS) time was measured from the dateof BNCT until confirmed death or the date of the last
follow-up exami-nation.
5HVXOWV: Median follow-up of surviving cases was 8.7months (range 0.9-29.8). At the time of analysis, 15 patients (62.5 %) were alive, and 9 patients (37.5%) out ofthem were alive with no evidence of disease. The local
recurrence was occurred in 12 patients, and a mediantime to recurrence was 4.8 months (range 2.7-15.4).
Nine patients died during an observation period, andeight of them died of disease progression. 1year OS andprogression free survival (PFS) rate was 50.0% (Fig 2.)
and 59.2% (Fig 1.), retrospectively. 1year OS rate of
ST group and non-ST group was 77.8% (median time
12.5 months) and 32.7% (median time 6.3 months) respectively (p=0.039) (Fig.3). 1year PFS rate of ST group
and non-ST group was 65.9 % (median time 11.6
months) and 25.0 % (median time 3.6 months) respectively (p=0.075) (Fig.4). There were no associations between the number of T/B ratio and OS rate, either PFS
rate. An addition of ST to BNCT did not increase any
adverse effects.
&RQFOXVLRQ: BNCT is effective in the treatment of locallyrecurred head and neck cancer.

0.5

11.5year&2 Establichment of a novel mutation breeding using Boron Neutron Capture Reaction (BNCR)
M. Kirihata, S. Segami1, Y. Hattori, Y. Kinashi2
5HVHDUFK&HQWHURI%1&72VDND3UHIHFWXUH8QLYHUVLW\
5HVHDUFK,QVWLWXWHRI(QYLURQPHQW$JULFXOWXUHDQG
)LVKHULHV2VDND3UHIHFWXUH,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: Boron Neutron Capture Reaction(BNCR) is based on the nuclear reaction of 10B atom withthermal/epithermal neutron already applied to cancer
treatment (BNCT) [1, 2]. As a new utilization method of
BNCR, the purpose of this study is to establish a novel
mutation breeding using BNCR.
This method uses the principle of inducing mutation by
an alpha particle and 7Li recoil nuclei high linear energy
transfer and short range when irradiated with neutrons(low energy thermal neutrons (< 0.5 eV) can be absorbed
the 10B atoms, leading to generating high linier energy
transfer alpha particles (~ 150 keV/μm) and 7Li nuclei (~175 keV/μm)) that are produced by BNCR of 10B selectively taken into the meristematic cell with thermal neutron. This principle is different from both chemical mutagens, such as EMS and MNU, and physical mutagens,such as gamma rays and ion beams, used for mutation
breeding so far. In other words, the mutagenic effect depends on chemical and physical factors, such as 10B concentration, thermal neutron intensity, and irradiation time.
The germination rate is used as one of the traits to verify
the effect of mutagenesis[3]. The immersed into BPA but
not irradiated with neutrons seeds were germinated normally at different concentrations (0, 10, 100, 200 ppm) of
BPA in the range of from 70% to 100%. This time, it was
confirmed that the germination rate was affected a thermal neutron fluence-dependent or a BPA concentration-dependent manner by causing BNCR.
EXPERIMENTS: The experimental material used Oryza sativa L. cv. Nipponbare. The dry seeds were immersed into different concentrations (0, 10, 100, 200ppm)
of 10B-enriched p-boronophenylalanine (BPA)[4] for 16 h.
Some concentrations were also tried with hulled rice. The
samples were washed with water and re-dried at room
temperature. The seeds in 2-mL tubes were irradiatedwith thermal neutron for 90 minutes in the Kyoto University Research Reactor (KUR). To provide four different levels of neutron fluence, the tubes were set to fourcolumns microtube rack at the time of irradiation. Afterthe irradiation treatment, the seeds were cultured in pe-tridishes with continual moistening of filter paper at 25Υ
under a photoperiod of 16 h light and 8h dark, it wasinvestigated the germination rate.

creased with both thermal neutron fluence and BPA concentrations (Table 1, 2). That is, the meristematic cell inthe seeds were not damaged enough to initiate cell division in the range of the present experimental conditions.
Besides, using hulled rice, the samples were fragile due
to re-drying. The hulled rice was not suitable for thismethod. We are set to confirm conditions for making astrong effect by making the fructose complex higher BPA
concentrations and extending the immersion time. By
investigating inhibition of germination and reduction insurvival of the samples, we will consider the suitableconditions as a mutagenesis method.

Table 2. The relationship between BPA concentrations and germination rate.
Concentrationsof BPA (ppm)

No. ofseeds

No. of seeds
germinatedgermination
rate (%)

germination
index
100

0

150

120

80

10

143

110

77

96

100

147

117

80

99

200

141

109

77

97

REFERENCES:[1] H. A. Soloway et al., Chem. Rev., 98 (1998),
1515-1562.
[2] B. Farhood, et al., Rep. Pract. Oncol. Radiother. 23(2018), 462-473.
[3] Tanaka A. et al., Int. J. Radiat. Biol., 72, (1997),
121-127.
[4] H. R. Snyder, et al., J. Am. Chem. Soc. 80 (1958),
835-838.

RESULTS: The typical thermal neutron fluence were
1.1x1013 cm2, 8.1x1012 cm2, 6.0x1012 cm2, 4.2x1012 cm2,at the time of irradiation. The germination rate not de-

31104

‑229‑

&2

(IIHFWVRQ'LVVHPLQDWLRQRU,QYDVLRQRIJOLRPDFHOOVE\%1&7

N. Kondo1, T. Kinouchi1, M. Natsumeda2, Y. Sakurai1, T.
Takata1 and M. Suzuki1,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ .8516
'HSDUWPHQWRI1HXURVXUJHU\%UDLQ5HVHDUFK,QVWLWXWH
1LLJDWD8QLYHUVLW\,1752'8&7,21  BNCT have been applied to recurrent malignant glioma and even after standard therapy(surgery, chemo-radiation therapy) because of the selective damage to the tumor. Especially, glioblastoma(GBM) is the most miserable cancer, whose patient survival is 14.6 months and remarkably resistant tochemo-radiation and immuno- therapy. With BNCT, we
achieved better local control and survival benefit in malignant glioma using thermal neutrons produced by thereactor in Kyoto University. However, the recurrence isinevitable after BNCT. Reasons for recurrence after
BNCT have not been fully elucidated, but they may reflect tumor characteristics. In fact, we’ve found cerebrospinal fluid dissemination, frequent cause of death, after
BNCT occurs more frequently in the small cell subtypeof IDH1R132H mutation-negative glioblastoma [1]. On
the other hand, exosomes, extracellular vesicles with diameter of between 50 nm to 150 nm used for communication tools between cells, are receiving a lot of attention
because containing microRNAs, lipids and proteins are
possible biomarker for various diseases. In this study, weinvestigate the exosomes from glioma cells after BNCT.
(;3(5,0(176
Cell culture: U87 MG glioma cells were cultured withexosome-free fetal bovine serum (FBS) at 10 % final
concentration in Dulbecco·s Modified Eagle·s Medium(DMEM) at 37 °C in 5 % CO2 incubator for two days.
Cells were divided into four groups, control, Boronophenylalanine (BPA) alone, thermal neutron irradiation
alone, and BNCT. BPA was added to the medium at 25
ppm the day before irradiation. One group consisted ofmore than 3×106 cells.
Thermal neutron irradiation: After trypsin treatment, cellsuspensions were divided in Eppendorf tubes at 1×106
cells/mL with exosome-free FBS at 10 % final concentration in DMEM with or without 25 ppm BPA and irradiated with thermal neutrons at D2O facility for one hour.
After irradiation, cells were centrifuged to change themedium, then dissociated into 10cm dishes with exosome-free FBS at 10 % final concentration in DMEM (1ð106
cells / dish).
Exosome isolation: 48 hours after irradiation, cell culture
medium (CCM) of each group was collected and centrifuged to remove the cell debris at 2000 rpm for 20 min at
4 °C. The supernatant was removed without disturbing
the pellet and filtered through 0.22 μm filters (Merck
Millipore) to remove contaminating remaining microvesicles, and cell debris and kept in – 80 °C deep
freezer.

After thawing, the CCM was concentrated to 500 Lwith Centrifugal Filter (Amicon Ultra-15, 100 kDa) devices at 4 °C. Following this, 500 L of CCM was overlaid on qEV size exclusion columns (IZon) and exosome
containing fractions were collected. Exosome fractions
were pooled and concentrated in Amcon Ultra-0.5 10 kDa
molecular weight centrifugal filter units to a final volumeof 50 L. Purified exosomes were then store at – 80 °C
until use.
Tunable resistive pulse sensing: The size distribution
profile and concentration of exosomes were analysedwith tunable resistive pulse sensing (TRPS) (qNano, Izon
Science Ltd). Carboxylated polystyrene beads (70 nm)
were used to calibrate the concentration and size.
5(68/76
The exosomes size distribution and concentration of eachgroup was assessed by TRPS. Exosome size from allgroups have the typical range of between 50 to 150 nm indiameter (Fig.1). Concentrations of exosomes of eachgroup: control, BPA alone, thermal neutron irradiation
alone, and BNCT, were 2.68 ×109, 1.89×108, 1.84×109,
1.18×108(/mL), respectively.
The contents of exosomes are to be analyzed by proteomics.

Fig. 1: TRPS analysis of exosomes confirming the size
range of 50-150 nm in diameter. (Arrows indicate eachgroup.)

5()(5(1&(6[1] Kondo N, HWDO, 2017, J Neorooncol. 2017;133:
107-118. doi: 10.1007/s11060-017-2408-x

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N. Kondo1, H. Fukusumi2, Y. Sakurai1, T. Takata1, Y.
Kanemura2 and M. Suzuki1
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ .8516
'HSDUWPHQW RI %LRPHGLFDO 5HVHDUFK DQG ,QQRYDWLRQ
5HVHDUFK 1DWLRQDO +RVSLWDO 2UJDQL]DWLRQ 2VDND 1D
WLRQDO+RVSLWDO

5()(5(1&(6[1] Fukusumi HWDO. (2018), Peer J,
DOI 10.7717/peerj.4187,1752'8&7,21  Biological effect of thermal neutron irradiation on neuron is unknown. Thermal neutron
is used for clinical treatment for Boron Neutron Capture
Therapy (BNCT). To avoid radiation brain necrosis after
BNCT, we investigate the pathway of cell death and inflammation induced by BNCT using human induced pluripotent stem cells (iPSCs)-derived neuronal cells.
(;3(5,0(176
Cell culture: We used human iPSC-derived Neural
stem/progenitor cell (NSPC) lines [1]. We differentiatedthese iPSC derived NSPCs and seeded into laminin-coated 8 well chambers and T25 flasks. Cells weresealed and transferred from the Osaka national hospital to
KURNS the day before irradiation kept at 24 °C in thebox and cultured at 37 °C CO 2 incubator after transfer.
Thermal Neutron Irradiation: We irradiated thermal neutron irradiation to these cells with sealing for 30 minutesat room temperature by D 2 O facility.
Cell death assay: We stained the cells in 8 well chamber
24 hour after irradiation with Hoechst 33342, Annexin
V-FITC and Propidium Iodide Solution following the
manufacture’s protocol (nacalai tesque, Japan) and captured them by the microscope [Keyence BZ9000].
Sampling for RNA isolation: We rinsed the cells in T25
flasks with PBS 24 hours after irradiation and lysed themwith QIAzol following the manufacture’s protocol (QIAGEN, Japan) and kept the cells at – 80 °C deep freezer.
5(68/76 We are still analyzing the results.

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N. Kondo1, E. Hirata2, M. Natsumeda3, Y. Sakurai1, T.
Takata1, and M. Suzuki1
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ .8516
'LYLVLRQRI7XPRU&HOO%LRORJ\DQG%LRLPDJLQJ&DQFHU
5HVHDUFK,QVWLWXWHRI.DQD]DZD8QLYHUVLW\
'HSDUWPHQWRI1HXURVXUJHU\%UDLQ5HVHDUFK,QVWLWXWH
1LLJDWD8QLYHUVLW\,1752'8&7,21  BNCT have been applied to recurrent malignant glioma and even after standard therapy(surgery, chemo-radiation therapy) because of the selective damage to the tumor. Especially, glioblastoma(GBM) is the most miserable cancer, whose patient survival is 14.6 months and remarkably resistant tochemo-radiation and immuno- therapy. With BNCT, we
achieved better local control and survival benefit in malignant glioma using thermal neutrons produced by thereactor in Kyoto University. However, the recurrence isinevitable after BNCT. Reasons for recurrence after
BNCT have not been fully elucidated. In this study, weinvestigate the crosstalk between tumor microenvironment cells and tumors which survive after BNCT.
(;3(5,0(176
Cell culture: We used mouse G261 glioma cell line andhuman glioma GBM1 line. Cells were cultured at 37 °C
in CO 2 incubator.
Xenograft model
Animals were anesthetized and immobilized in a small
animal stereotactic device. 2105 cells were transplanted
through a hole 2 mm to the right of the bregma, at a depthof 3 mm, at a rate of 1 micro L/min. G261 were transplanted to C57BL/6J mice and G261 were transplanted toBalb/cA-nude mice.
Boronophenylalanine (BPA) Treatment and Thermal
Neutron Irradiation: After 10 days from transplantation,
500mg/kg of BPA was administrated subcutaneously 1hour before irradiation. We irradiated thermal neutron tothese mice shielding body trunk with lithium fluoride for
15 minutes at room temperature by D 2 O facility with
5MW power.
Sampling for Immunohistochemistry: 48hours and 7 days
after irradiation, mice were anesthetized and sacrificed
after transcardiac perfusion of PBS and 4 % paraformaldehyde (PFA). The brain tissue was removed and fixedwith 4% paraformaldehyde overnight, then transferred to
30 % sucrose in PBS. The tissue blocks were frozen at ²
80 °C.
5(68/76 We are still analyzing the results.

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M. Suzuki, H. Tanaka, Y. Tamari, T. Watanabe, S. Takeno1,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  In the process of ARG, we need toacquire tissue staining image and etched pit image separately and merge them using its markers. So precise marking system is the essential for precise analysis. But in the
etching process, ordinary markers using ink are easily disappeared. To avoid disappearing the markers, we usedscratch markers on the CR-39 since scratch remains afteretching process [1].
However, in chemical etching process, scratch marker isalso etched, and the marker become larger. Because theshape of the marker is deferent before and after etching,
the preciseness of matching image is not good enough.
In this study, we devised new marking system, of which
the marker deformation before and after etching is minimal by keeping the marker away from the etching solution.
Here, we report the method of the newly devised marking
system and the assessment the precision of it.
(;3(5,0(176 The process of ARG using newly devised marking system is shown as bellows.
1. Put the tissue section on the CR-39 and irradiate themwith thermal neutron.
2. Put small marker using ball-point pen near the place tobe analyzed, on the opposite side of tissue section.
<Fig.1>
3. Put the CR-39 on the slide glass using epoxy adhesives,
which has good chemical resistance. In this process,the marker should be inside between CR-39 and slide
glass. <Fig.2>
4. Stain the tissue section and acquire both tissue image
and corresponding marker image using optical microscope.
5. Remove the tissue section from the CR-39.
6. Etch the CR-39 chemically and acquire both the etched
pit image and corresponding marker image.
7. Merge two images (acquired in process 4 and 6) using
its markers.

<Fig.1>Marker deformation before and after chemical etching We defined maximum deformation length (dL) between
before and after etching marker as bellows.

݀‫ ܮ‬ൌ  ඥ݀‫ ݔ‬ଶ ൅ ݀‫ ݕ‬ଶ
dx: size difference of horizontal direction
dy: size difference of vertical direction
 The maximum deformation length means maximum potential error in matching images using the markers.
 Five samples are assessed.
5(68/76 The maximum deformation length of eachmarking method is shown as bellows. The average maximum deformation length is 6.17um and 0.39um for scratchmarker and newly devised marker, respectively.
([DPSOHRIHDFKPDUNHU

5()(5(1&(61. H.Tanaka HWDO -5DGLDW5HV , (2014) 373–380<Fig.2>In the experiment, we used CR-39 (BARYOTRAK) andacquired their images using microscope (Keyence BZ9000). Automatic marker matching program was created
and tested.

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Y. Sakurai, H. Matsunaga1, T. Takata, H. Tanaka, M. Suzuki

cal region of 5 cm in diameter was settled in the phantom.
This region was modelled after a tumor part, and its boron concentration was 250 ppm. The standard epi-thermal
neutron irradiation mode was used for this experiment.
For the positions of the first and second collimators, theprompt gamma-rays due to 10B(n,αγ)7Li and 1H(n,γ)2D
reactions were counted by the high-purity germanium(HPGe) detector settled on the irradiation room ceiling.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\,1752'8&7,21 Whole organ irradiation in radiotherapy is effective on multiple tumors and minimal residual tumors, such as whole brain irradiation for brain
metastasis, whole conserved-breast irradiation in conservative therapy for breast tumor, etc.. However, it cannot be realized for liver and lung tumors. It is because thetolerant dose of these organs is 20 to 40 Gy, which issmaller than the tumor control dose of 50 to 80 Gy. In
BNCT, the ranges of the heavy charged particles due tothe 10B(n,αγ)7Li reaction in the boron compound, which
selectively accumulates in tumor cells, are too short toreach the adjacent normal cells. Therefore, BNCTs withthe whole organ irradiation for liver and lung tumors canbe realized as radiotherapy.
In BNCT clinical studies for liver and lung tumors at
KUR, the equivalent doses for normal liver and/or lung
have been estimated on the basis of boron concentrationin blood, which is measurable by prompt gamma-ray
analysis. But actually, the variation for the boron concentration in normal liver and/or lung is assumed to be larger
among the patients with basal disease, such as cirrhosis,
pulmonary fibrosis, pulmonary emphysema, etc..
The purpose of this research is the development of thereal-time boron-concentration estimation system in liver
and/or lung during BNCT, in order to improve the dose
estimation accuracy for BNCTs with the whole-liver
and/or whole-lung irradiation. In this system, the technique of prompt gamma-ray telescope is applied. A
gamma-ray telescope system has been in use for liver
tumor BNCT at Heavy Water Neutron Irradiation Facilityof KUR (KUR-HWNIF) from 2005 [1]. The collimation
system of this telescope was improved in 2017.
An experiment was performed to confirm the basic characteristics of this improved telescope system in 2019.
0(7+2'6 Figure 1 shows the outline of the original
gamma-ray telescope system. A 100 cm-long collimatoris located in the hall through the irradiation-room ceilingwall. The first collimator is settled just before the detector,
and the second collimator is settled at the bottom of thecollimation system. In the improved system, both collimators are placed in the collimation system. The distance
between these collimators is changeable.
The layout of the characterization experiment was almost
similar to the layout in Fig. 1. Instead of a patient, awhole-body liquid phantom was placed. This phantom
was the 1-cm-thick acrylic case filled with boric acidwater. The boron concentration of the boric acid water
was 25 ppm for boron-10. A higher-concentration spheri-5(68/76 Figure 2 shows the ratio of the prompt
gamma-ray counts of boron-10 to hydrogen-1 for thecollimator interval. In this case, the collimator position issettled to be highest, and the second collimator moves
from the highest position to the lowest position. As thesecond collimator position is lower, the collimator interval is larger and the telescope FOV is smaller. As shownin Fig.2, the count ratio is smaller as the collimator interval is larger. This reason is considered to be the influenceof the position of the higher-concentration region in thetelescope FOV. It is thought that the higher-concentration
region gradually goes out from the telescope FOV, according to the increase of the collimator interval.
&21&/86,21 The basic characteristics of the improved telescope system were experimentally confirmed.
The further analyzation of the experimental data and the
additional experiments are planned.
$&.12:/('*(0(176 This study was supported by The Kyoto University Research Fund (Core Stage
Back-up, in 2017).

Fig. 1. Outline of the original gamma-ray telescope
system installed at KUR-HWNIF.

Fig. 2. Ratio of gamma-ray counts for B-10 to H-1.
5()(5(1&(6[1] Y. Sakurai HW DO, Appl. Radiat. Isot.  (2004)
829-833.

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I. Ota, H. Uemura, A. Nishimura, T. Kimura, S. Mi-kami,
T. Yamanaka, M. Suzuki, Y. Sakurai, H. Tanaka,N.
Kondo, T. Tamamoto, M. Hasegawa and T. Kitahara'HSDUWPHQWRI2WRODU\QJRORJ\+HDG 1HFN6XUJHU\'HSDUWPHQWRI5DGLDWLRQ2QFRORJ\1DUD0HGLFDO8QL
YHUVLW\
,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 Neutron capture therapy (BNCT)
for head and neck tumors has been clinically studied
since 2001, with the BNCT research group at Kyoto
University Reactor Laboratory, which is a co-investigator,
highly effective, with high safety. It is being established.
Since November 2012, we implemented the therapy as a
joint research with Kyoto University Reactor Laboratory,
with the consent of the patients in 4 cases of refractory
recurrent head and neck cancer. As a result, the response
rate was a very high 100%. The tumor reduction effect inrecurrent cases after radical irradiation, which could not
be achieved by conventional treatment methods, strongly
suggests the possibility of expanding the indications for
BNCT for refractory carcinomas as well as for head andneck cancer cases. Here, we will perform BNCT for refractory and recurrent head and neck tumors and examine
their efficacy and optimal protocol.
(;3(5,0(176 We will treat BNCT for refractoryand recurrent head and neck tumors that meet the following criteria and examine their efficacy and optimal
protocol.
Inclusion Criteria

Exclusion Criteria(1) The patient with active multiple primary cancers;
synchronous or metachronous (within 5 years) double
cancers .
(2) The patient with metastatic lesion.
(3) The patients with severe complications.
(4)The patients with infection requiring systemic treatment.
(5) The patient with severe adverse event(>Grade3, CTCAE v4.0) in the BNCT region.
(6) The patient with cardiac pacemaker.
(7) The patient judged to have difficulty in maintain posture during the protocol treatment.
(8) The patient with WBC; < 3000/mm3, PLT; <100000/mm3(9) The patient with recurrence lesion invasive to carotid
artery and toskin.
(10) Patients with phenylketonuria.
5(68/76 We enrolled one patient and undertook
BNCT during this period as follows:
Patient #1: 46 y.o. female
Recurrence of cancer of the external ear
Histology: squamous cell carcinoma
Effect: SD
SAE: none; dermatitis, Grade 2&21&/86,21
We will continue to accumulate the cases carefully toestablish a safe and stable treatment of BNCT.

(1) The patient with local recurrence of head and neckcancer who can not perform the standard therapy any
more after radiotherapy.
(2) The patient with local recurrence of head and neckcancer by the imaging diagnosis, such as CT, MRI and
PET.
(3) The patient with previous radiotherapy (total 40-75
Gy, 2Gy/fq) for the recurrent region.
(4) The patient with the period of more than one monthsince the previous treatment.
(5) The patient with recurrence lesion in the less than
6cm of depth from skin as GTV for BNCT.
(6) The Patients who have PS less than 2 and are expected to survive more than 6 months after BNCT.
(7) The patient with good condition of renal function:
creatinine <1.2 mg/dl for male and<1.0 mg/dl for female.
(8) The patient with the age between 20 and 80.
(9) Written informed consent with one own will.

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

'HSWRI1XFOHDU(QJLQHHULQJ 0DQDJHPHQW6FKRRORI(QJLQHHULQJ 8QLY RI 7RN\R 'HSW RI %LRHQJLQHHULQJ
6FKRRORI(QJLQHHULQJ8QLYRI7RN\R &RRSHUDWLYH8QLW
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9HWHULQDU\ +RVSLWDO 'HSW RI +XPDQ  0ROHFXODU 3D
WKRORJ\*UDGXDWH6FKRRORI0HGLFLQH7KH8QLYHUVLW\RI
7RN\R 2VDND &LW\ 8QLYHUVLW\ *UDGXDWH 6FKRRO RI(QJLQHHULQJ ,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
Neutron Capture Therapy(NCT) is a nonsurgical therapeutic modality for treating locally invasive malignant
tu-mor. Basically, there are boron NCT and Gadolinium
NCT. Considering the possibility of MRI-guided
GdNCT be-cause gadolinium compound is a kind of
MRI contrast agent [1], we focused on GdNCT.
However, clinical Gd-chelates lack high and selective
accumulation in tumors for electing safe and potent
GdNCT [2].
Recently, nanoscale drug becomes more and more
pop-ular because it can promote the accumulation of Gd
agents in tumor through the enhanced effect of
permeability and retention (EPR). Therefore, we built aseries of nanocarri-ers to improve the accumulation intumor and evaluated its antitumor effect through thecomparison of tumor size.
(;3(5,0(176First of all, a series of nanocarriers based onpoly(aspar-tic acid) (P(Asp)) were developed and they
were modified with poly(ethylene glycol) (PEG) chainsin order to have different molecular weight (Mw). And
then, through the introductionof
Gd-DOTA,
PEG272(PEG272-P(Asp-Gd-DOTA))
andPEG454(PEG454-P(Asp-Gd-DOTA)) were made as the
final products.
After 24h injection into colon 26 tumor-bearing
mice with PEG272 and PEG454, respectively, the tumorbearing mice received neutron irradiation 60 minutes at
Nuclear Reactor Facility of Kyoto Univ Institute forIntegrated Ra-diation & Nuclear Science with average
neutron fluence of 2.0 × 1012 n/cm2. Moreover,considering the influence of irradiation, we also set themice injected same samples but without receiving
irradiation as controls groups.
After almost one-month observation, the situation of
all mice was recorded and the conclusion about
antitumor ef-fect was showed below according to thetumor size com-parison photos.

From the photo of tumor size after one-month observation, we can easily know that compared with the control
group, tumor growth was suppressed with the injection ofsamples and according to the comparison in the control
group, the suppression worked not only through the irradiation, but the influence of samples. Especially in the
PEG272 group, the tumor almost disappeared after irradiation which indicated the excellent tumor suppression ability of PEG272.

:LWKLUUDGLDWLRQ /HIW :LWKRXWLUUDGLDWLRQ 5LJKW 
3(*JURXS:LWKLUUDGLDWLRQ /HIW  :LWKRXWLUUDGLDWLRQ 5LJKW 
3(*JURXS:LWKLUUDGLDWLRQ /HIW :LWKRXWLUUDGLDWLRQ 5LJKW &RQWUROJURXS
7DEOH7XPRUJURZWKVXSSUHVVLRQE\*G1&7XVLQJ
3(*3(*
5()(5(1&(6[1] A. Narmani HWDO. J. Drug Deliv. Sci. Technol.,  44,457466
[2] H. Tokumitsu et al. Pharm. Res. 1999, 16, 1830–1835

5(68/76

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M. Ishikawa1,2, H. Handa2, K. Baba2, K. Takamiya3 and
Y. Sakurai3

Table 1
Probe
1
2
3
4



)DFXOW\RI+HDOWK6FLHQFHV+RNNDLGR8QLYHUVLW\*UDGXDWH6FKRRORI%LRPHGLFDO6FLHQFHDQG(QJLQHHU
LQJ+RNNDLGR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 In the conventional BNCT, thermal
neutron flux and thermal neutron fluence during treatment could not be measured in real time because gold
wire activation was used to evaluate thermal neutron fluence. Therefore, we developed a detector (SOF detector;
Scintillator with Optical Fiber Detector) with a plastic
scintillator attached to the tip of the optical fiber, tried
real-time measurement of thermal neutron flux in neutron
capture therapy, and got good results. The long-term stability of the SOF detector and the wide measurement dynamic range (linearity of 104 to 1010 n/cm2/s) have been
confirmed in previous collaborative experiments. [1,2]
However, signal degradation of SOF detector inlong-term exposure was reported [3]. The signal degradation might not be a significant problem in case that calibration can be performed before use. However, signal
degradation greatly affects measurement accuracy in caseof long-term monitoring because calibration prior to use
is difficult. In previous experiment performed at last academic year, we tried to identify the causative substance of
signal deterioration of the material in the SOF probe,
however, it was difficult to specify the caused material
because the amount of signal deterioration was not sufficiently large at Heavy Water Neutron Irradiation Facility(HWNIF). Therefore, we conducted a deterioration characteristic assessment in a high flux environment.

Probe characteristics.
Neutron conv.
6LiF
6

LiF
-

Reflector
BC642
BC620

Slope [%/n㺃cm-2]-2.38×10-14-4.55×10-14-3.26×10-14-4.53×10-14

5(68/76 Figure 2 shows the relative change for eachprobe from the initial signal intensity at irradiation start.
From Fig. 2, the signal intensity is greatly attenuated with
the irradiation. The slope of signal deterioration assuming
attenuated linearly was shown in Table 2. With respect tothe thermal neutron dose of 1014 n/cm2, it was confirmedthat the probe mixed with the neutron converter showed~3% attenuation, and the probe containing no neutron
converter had 4.5% attenuation. Usually, neutron fluenceof ~1013 n/cm2 is irradiated in BNCT treatment, so it isestimated that signal deterioration during treatment is lessthan 0.5%. On the other hand, according to the report ofNakamura HW DO, the deterioration of the plastic opticalfiber is considered to be a major factor because the damage caused by irradiation was reduced by constructing
SOF detector probe with a quartz optical fiber.[4] Our
result that the signal deterioration was confirmed regardless of the presence or absence of the neutron converter isconsistent with the report of Nakamura HWDO.

(;3(5,0(176 The experimental geometry is shownin Fig. 1. The Slant exposure tube (SET) facility SET of
KUR was used for irradiation. The SOF detector probes
were arranged at about 50 cm above from the bottom of
Slant hole where estimated thermal neutron flux was
4.68×1010 n/cm2/s with 5 MW operation. The combinations of neutron converter and reflectors contained in theirradiated probes are shown in Table 1. All probes used
BC490 as a plastic scintillator, and Probes 1 and 2 weremixed with 6LiF as a neutron converter. Moreover,BC642 (PTFE Reflector Tape) and BC620 (Reflector
paint) were used as a reflective material.

(a) Normalized at initial signal intensity.

(b) Normalized with probe #4.

Fig. 2.

Irradiation geometry for on-line assessment of deterioration characteristics.

5()(5(1&(6Fig. 1.

Irradiation geometry for on-line assessment of deterioration characteristics at Slant exposure tube.

>@ M. Ishikawa HWDO, Appl. Radiat. Isot.,  (2004) 775-779
>@ M. IshikawaHWDO, Nucl. Instr. Meth., A  (2005) 448-457
>@ M. KomedaHWDO, Appl. Radiat. Isot.,  (2009) 254-257
>@ T. NakamuraHWDO, J Radiat. Prot. Res.  (2016) 105-109

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0HDVXUHPHQWVRIPXOWLSKDVHIORZG\QDPLFVXVLQJQHXWURQUDGLRJUDSK\Y. Saito and D. Itoment error in the film thickness shall be quantitively estimated by improving the imaging system and processing
method.

,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Neutron radiography (NRG) is a
powerful tool for multiphase flow visualization as well as
ordinary fluid dynamics. As one of the applications of
NRG, gas-liquid two-phase flows in a metallic pipe havebeen clearly visualized by using NRG. However, themeasurement accuracy of thin liquid film formed in such
two-phase flows has not been fully evaluated. The liquidfilm thickness is one of the important parameters to investigate the two-phase flow behavior. In this work, ourneutron imaging system has been modified to realize
more sophisticated flow visualization and precise measurements of thin liquid film

Fig. 1'(9(/230(17 2) +,*+63((' 1(87521
,0$*,1* 6<67(0 A high-speed neutron imaging
system for flow visualization has been developed at theB-4 supermirror neutron guide facility [1] of the Institutefor Integrated Radiation and Nuclear Science, Kyoto
University. This imaging system consists of a neutron
converter, a dark box with a single mirror, an ultrasensitive lens, an optical image intensifier and a high-speed
camera. The high frame rate up to 10,000 frame/sec could
be achieved using above-mentioned combination at theB-4 port [2]. The pixel resolution and frame rate can be
adjusted by selecting the optics.
9,68$/,=$7,21 2) 6,08/$7(' 7+,1 ),/0
Neutron imaging experiments were conducted at the E-2
port of the Kyoto University Research Reactor. In thisport, the neutron flux is 1×105 n/cm2s, and the beam size
is 15 cm in diameter. CCD camera system was employed,
and the static film thickness was estimated from the neutron transmission images. As a preliminary work, theliquid film formed in two-phase flows was simulated by
the thin polyimide sheet and the thickness was varied
from 75 μm to 250 μm. The polyimide has the macro-

0 degree15 degrees

30 degreesg

45 degreesg

60 degreesg

75 degreesgFig. 2 Neutron transmission images of polyimide
sheet (į = 250 μm).

Neutron transmission>@1.00

scopic neutron cross-section of 1.3cm-1. The film sample and rotation stage are shown in Fig.1. The angle ofthe polyimide film was set at 0~75 degrees. The neutron transmission images of the polyimide film withthe thickness of 250 μm are shown in Fig.2. At smaller
angle conditions, there is little change in the transmission. However, at the angle of 75 degrees, the neutron
attenuation changes obviously. The mean value of theneutron transmission in the polyimide film area is plottedin Fig.3, and they are compared with the results of geometric calculation. Most of the results show good agreement, however, some measured results with the transmission values larger than 0.98 depart from the calculation
results. It would be suggested that the estimation of verythin film should be a challenging problem in present neutron imaging technique. In the next step, the measure-Sample and rotation stage.

0.95

0.90

Calc.

Exp.
75Pm
125Pm
250Pm

0.85

0.80

0

10

20

30

40

50

60

70

80

Angle>GHJ@Fig. 3

Angle dependence of neutron transmission.

5()(5(1&(6[1] Y. Saito, HWDO., Nucl. Instr. Meth. Phys. Res., A, (2011) 36-41.

31034

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9LVXDOL]DWLRQRI+\GURJHQLQ3XUH3DOODGLXPYLD1HXWURQ5DGLRJUDSK\DQG
7RPRJUDSK\K. Shimizu1, H. Toda2, K. Hirayama2, H. Fujihara2, D.
Ito3, Y. Saito3
'HSDUWPHQW RI 3K\VLFDO 6FLHQFH DQG 0DWHULDOV (QJLQHHULQJ,ZDWH8QLYHUVLW\
'HSDUWPHQW RI 0HFKDQLFDO (QJLQHHULQJ)DFXOW\RI (Q
JLQHHULQJ.\XVKXXQLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  It is widely recognized that hydrogen in metallic materials degrades the mechanicalproperties of the materials. Various hydrogen embrittlement mechanisms, such as HELP, HEDE and HESIV
have been proposed to date [1], but there is still no comprehensive interpretation. However, for each mechanism,
it is consistent that hydrogen trapping and the resulting
localization of hydrogen to defects and microstructures
are the dominant factors of hydrogen embrittlement [2].
To understand the hydrogen embrittlement, it is necessary
to visualize the hydrogen distribution and to elucidate its
evolutionary behavior over time. In this study, hydrogenin a metal was visualized by neutron radiography andtomography, and hydrogen accumulation under stress wasassessed. Several palladium specimens with differenthydrogen contents were prepared and a notch was introduced. It has been demonstrated that hydrogen content
can be analyzed by neutron tomography, and the possibility of evaluating hydrogen accumulation under stress is
discussed.
(;3(5,0(176 Palladium specimens with hydrogencontents of 0 at%, 10 at%, and 20 at% were prepared forneutron imaging. Hydrogen content was controlled byhigh temperature hydrogen exposure. Neutron radiography was performed on the KUR E-2 port [3]. The imaging system consists of a 6LiF:ZnS visible light converter and a cooled CCD detector. The exposure time was
set to 5 min at a thermal power of 1 MW in the research
reactor. Neutron tomography was also performed at the
KUR E-2 port. A rotating stage for tomographic observation was added to that of radiography. Neutron transmission images were obtained by rotating the specimen from0 to 180° in 1° increments. Total 180 images were reconstructed in a 3D image using a convolutional back projection algorithm.
5(68/76 Fig. 1 shows tomographic cross-sectional
images of the central part of specimens before and after
tensile loading. Fig. 1(d) shows the profile of CT value
obtained from the white lines in Fig. 1(a-c). The contrast
between 0%H and 10%H at no load indicates that thedifference in hydrogen content can be evaluated fromimage contrast as well as the transmission image. On theother hand, no hydrogen accumulation was observed
when comparing before and after tensile loading at 10%
H. The location of [ = 3 mm in Fig. 1(d) corresponds tothe notch tip of specimen, but the change in hydrogencontent before and after loading could not be measured
even in the line profile. This was true not only at the center of specimens shown in Fig. 1(a-c), but also near thesurface. The notch opening displacement was measured
to be about 510 Pm. The plastic zone size of the notch tip
was calculated to be about 220 Pm by estimating the applied stress of the specimen from the opening displacement. It is inferred that the hydrogen accumulation isremarkable in this region. The measured tomographic
image has a resolution of about 400 Pm. This suggest thathydrogen accumulation was not visualized in Fig. 1(c)and (d), because of accumulation region was smaller than
400 Pm. It is expected that short-time 3D imaging with aspatial resolution of 200 Pm is available by upgrading theimaging system. Using this system, 3D/4D analysis ofhydrogen accumulation behavior will be revealed byneutron tomographic observation.
5()(5(1&(6[1] I. M. Robertson HW DO, Metall. Mater. Trans. A 46
(2015) 1085-1103..
[2] Z. Zhang HWDO, Acta. Mater. 113 (2016) 272–283.
[3] Y. Saito HW DO, J. Jpn. Soc. Precis. Eng. 79 (2013)
822–825.
[4] K. Shimizu HWDO, J. Japan Inst. Met. Mater. 83 (2019)434–440.

31036

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Fig. 1. Virtual cross-sections of the 3D neutron
tomographic images; (a) palladium without hydrogen, (b) that with 10 % hydrogen, and (c) that with
10 % hydrogen after loading. (a) and (b) were observed without loading. (d) Line profiles obtained
from the white solid lines in (a~c).

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LQ3DUDOOHO0LQLFKDQQHO+HDW([FKDQJHU

H. Asano, H. Murakawa, R. Moriyasu, S. Inoue, K.
Sugimoto, D. Ito1DQG Y. Saito1'HSDUWPHQWRI0HFKDQLFDO(QJLQHHULQJ.REH8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
Microchannel compact heatexchangers are paid attention for the compactness andreduction in temperature difference between fluids. Since
smaller diameter leads to larger pressure loss, microchannel heat exchanger has many parallel channels.
Therefore, in the case that the heat exchanger is used forevaporator, refrigerant flow distribution often causes a
deterioration in the heat transfer performance. In thisstudy, boiling flow behaviors in a single layer
microchannel heat exchanger had been visualized byneutron radiography, and void fraction distributions had
been measured from the radiographs.
(;3(5,0(176 The tested heat exchanger was
manufactured by diffusion bonding of thin stainless steel
plates, and consists of single-layer refrigerant and heating
medium parallel channels. The channel cross-section andflow arrangement are shown in Fig. 1 and 2, respectively.
HFC-134a and FC3283 were used as the refrigerant andthe heating medium, respectively. The number ofchannels are 21 for the refrigerant and 20 for the heating
medium. Each channel has semicircular cross-section.
The heat exchanger was placed in vertical plane to form
vertically upward boiling flows of the refrigerant. To
avoid maldistribution of refrigerant flows, two kinds ofdivided ribs, such as perforated and offset types, as
shown in Fig. 3 are used. Radiographs were recorded bya cooled CCD camera with the exposure time of 30
seconds and the pixel size of 88 Pm/pixel.
5(68/76 Void fraction was measured for each pixel ofvisualized images, and the distributions for the test
sections with the straight parallel channels, the perforated
and offset type channels of refrigerant are shown in Fig. 4(a) to (c), respectively. It can be clearly observed that thevoid fraction on the right side close to the heating
medium inlet was higher than the left side due to thelarger temperature difference. It was seemed that void
fraction distribution became more homogeneous for the
perforate rib. In this case, the inlet condition ofrefrigerant was a subcooled liquid. The onset of boilingmight affect the flow distribution. For the perforated type,the holes through the ribs might help bubble nucleationand development of two-phase flows.

(a) R134a(b) FC3283
Fig.1
g Channel cross-section

Fig. 2 Flow arrangement(a) Perforated type(b) Offset typeFig. 3 Rib pattern in refrigerant channel

Void fraction

1.0

R134a
R134a
R134a
(a) Straight parallel channels(b) Perforate rib(c) Offset rib
Fig. 4 Void fraction distributions (mass flux : 150 kg/(m2㺃s) for R134a, 920 kg/(m2㺃s) for FC3283,
LQOHWWHPSHUDWXUHႏIRU)& 

31045

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0

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H. Murakawa, S. Torii, K. Mine, K. Sugimoto, H. Asano,
D. Ito1 and Y. Saito1*UDGXDWH6FKRRORI(QJLQHHULQJ.REH8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Water management is a key topic
of a polymer electrolyte fuel cell (PEFC). If condensed
water exists in the gas diffusion layer (GDL) and the gas
channel, it may depress the gas diffusion as flooding.
Furthermore, loss in electric power generation in PEFCs
is due to resistances such as ionic, activation, concentration, etc. Many of these resistances are related to themass transport in the PEFC. To evaluate the resistances ina PEFC, electrochemical impedance spectroscopy (EIS)
has been widely used [1]. However, the effect of water in
the PEFC on the resistances has not been fully understood. Aim of this study is to clarify the effect of water in
the PEFC on the resistances. Simultaneous measurementsof the water distribution and the electrical impedancewere carried out by using neutron radiography and EIS.
Changes in water accumulation in the PEM and the GDL
were compared with the resistances.

distributions at 9 and 15 min is not significant for L = 316
mA/cm2. Therefore, it can be confirmed that the water
distributions are almost steady states after 9 min. On theother hand, water gradually accumulated in the channel
for L =500 mA/cm2. The water accumulation at downstream channel, LH 6th channel, is greater than that at 4th
channel. This is because the relative humidity becomes
higher at downstream position, and the water accumulation is easy to occur.
Fig. 2 represents change of the reaction resistance, 5CT.
5CT gradually decreases until 15 min at L = 316 mA/cm2.
For L = 400 mA/cm2, 5CT gradually decreases until 9 min,and it became almost constant after the time. Furthermore,
it gradually increases after 2 min for L = 500 mA/cm2. As
confirmed from the water distribution, the much water
accumulation was confirmed in the channel. This preventthe water supply to the GDL resulting in increases of theconcentration resistance. However, the effect was not
significant although water accumulation was clearly confirmed in the channels at 15 min for L = 500 mA/cm2.
Water thickness [μm]1500

Anode Cathode(;3(5,0(176 A small size PEFC having a single-serpentine gas-channel with cross-sectional area of 1
× 1 mm2 was used for measuring two-dimensional water
distribution and the electrochemical characteristics.
Nafion® NR-212 was used as the PEM with a thicknessof approximately 90 μm having catalyst layers on boththe anode and cathode sides. The GDL was carbon paper(Toray Ind.) with thickness of 190 μm at the cathode sideand 280 μm at the anode side. The porosity of the GDL
was approximately 78%. Two-dimensional water distributions were obtained every 60 sec during the PEFC operation. The EIS measurements were simultaneously carried out with the neutron radiography for evaluating the
PEM resistance and the reaction resistance, 5CT [Ω]. Thehydrogen and air flow rates were 84 and 196 cc/min, respectively. The experiments were carried out at room
temperature, while the temperature of the PEFC varied
between 25 – 30 °C

9 min
15 min9 min
15 min(a) L = 316 mA/cm2(b) L = 500 mA/cm2
Fig. 1. Two-dimensional water distributions

Reaction resistance, 5CT [m:]5(68/76 Two-dimensional water distributions atcurrent density L =316 and 500 mA/cm2 are compared in
Fig. 1. Measurement area is between 4th and 6th channels,
and the top channel in the figure is the upstream position.
Liquid water accumulation during the PEFC operation
can be confirmed as indicated by the gray-scale. The time
represents the elapse time from the power generation.
Amounts of water accumulation in the GDL under thelands and channels are different and a large amount ofwater existed under lands at the earlier results. It indicated that water accumulation is started under the lands.
Then, liquid water reaches channel and are particularly
concentrated on the land corners. Difference of the water

0

500
400
300
200

316 mA/cm2
2
400 mA/cm
2
500 mA/cm

100
0

5

10
Time [min]15

Fig. 2. Time-series of the reaction resistances.
5()(5(1&(6>@ E. Antolini, et al., J. Power Sources,  (1999)
142.

31046

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Flow visualization of heavy oil in supercritical water using neutron radiography

T. Tsukada, M. Kubo, E. Shoji, N. Ito, T. Kaneko, S. Kodaira, S. Takami1, K. Sugimoto2, D. Ito3, Y. Saito3
Dept. of Chemical Engineering, Tohoku University
1
 Dept. of Materials Science and Engineering, Nagoya
University2
Dept. of Mechanical Engineering, Kobe University
3
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
INTRODUCTION: With an increase in the demandfor petrochemical feedstock and middle distillate, utilization of heavy oil such as atmospheric or vacuum residue
is also necessary. Since the heavy oil has high viscosity
and its quality is low, desulfurization and upgrading processes are required to use the heavy oil effectively. Insuch a situation, upgrading process using supercriticalwater has been proposed and studied recently.
Understanding of flow behavior of heavy oil in reactors filled with supercritical water is important to improve the performance of upgrading process. However,the phenomena are too complicated to simulate numerically. Since, in experiment, the reactor is made of metalfor operation at high pressure and high temperature, thevisualization using visible light is not available. Thus, thenumerical simulation and experimental flow visualizationof heavy oil flow in supercritical water have not been
conducted. In our previous study [1], we have visualized
the heavy oil flow in a trickle bed reactor under N2 atmosphere using neutron radiography, and indicated thepotential of neutron radiography to investigate the flow
behavior of heavy oil. Therefore, as a next step, the visualization of the heavy oil behavior in supercritical waterby neutron radiography was carried out, continuing fromlast year.
EXPERIMENTS: In neutron radiography for the flow
visualization of heavy oil in supercritical water, the Kyoto University Research Reactor (KUR) was utilized as
neutron source. A series of neutron radiography experiments was conducted with a thermal neutron flux of
8.5×107 n/(cm2∙s).
The reactor consists of a 1/2-inch stainless steel tube
filled with Al2O3 particles with a diameter of 3 mm. The
heavy oil, i.e., atmospheric residue (AR), was supplied toa reactor from above with the flow rates of 2.5 or 5.0
g/min. On the other hand, the water was supplied counter-currently with the flow rates ranged from 0.05 to 7.5
g/min. The reactor was heated to temperatures of 400°C
and was operated at 25 MPa.
An image intensifier and a camera at the framerateof 30 fps were used to obtain radiography images of theunsteady flow behavior. An image processing to reducenoises and to calculate neutron attenuation was performed for the obtained radiography images.
RESULTS: The flow behavior of heavy oil in the reactor varied depending on the experimental conditions

were visualized using neutron radiography. Fig. 1 shows
the time variation of flow behavior of heavy oil in supercritical water at the flow rates of heavy oil ( Zo) and water(Zw) were 2.5 g/min and 0.05 g/min, respectively.
Fig. 2 shows the variations in the area-averaged
neutron attenuation ( PUd ) over time, which were calculated over the 8 mm (40 pixels) u 40 mm (200 pixels) area
shown in the inset of Fig. 2 under the four experimental
conditions. The area-averaged neutron attenuation increased with time and reached a constant value under all
the tested conditions. The time required to reach a constant attenuation became longer with increasing supercritical water flow rate, particularly at Zo = 2.5 g/min. In
addition, Case D shows the increase in the attenuation
after 40 s due to the upward flow of heavy components ofoil from the bottom of the reactor.
CONCLUSION: The results obtained by neutron radiography showed that the flow behavior of heavy oil in thepacked bed reactor under supercritical water environment
depends on the flow rates of heavy oil and supercriticalwater.

Fig. 1: Flow behavior of heavy oil in supercritical water
when the flow rates of heavy oil and water were 2.5
g/min and 0.05 g/min, respectively. μ, ρǡd are massattenuation coefficient of thermal neutrons [m2/kg], density of heavy oil [kg/m3], and thickness along the neutron
beam direction [m].

Fig. 2: Time variations of area-averaged neutron attenuation.
REFERENCES:[1] E. Shoji et al., Chem. Eng. Sci., 196 (2019) 425-432.

31074

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60

120

180

Time (sec)

240

300

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Fig. 3. Moisture and temperature profile evolution at
different depths from the heating surface

31103

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&2'HYHORSPHQWRIFDSLOODU\SODWHEDVHGIORXUHVFHQWSODWHVIRUQHXWURQUDGLRJUDSK\T. Sakai1, K. Kurita1, H. Iikura1, D. Ito2, Y. Saito2


0DWHULDOV6FLHQFHV5HVHDUFK&HQWHU-DSDQ$WRPLF(Q
HUJ\$JHQF\
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Fluorescent plates are widely used
for neutron radiography. In the case of the imaging devices, the spatial resolution of fluorescent plates conflicts
with their detection efficiency. In general, a thicker
phosphor layer increases the efficiency, but adversely
affects the resolution because of blurring [1]. In this work,
we developed a new approach to fabricate micro-structured fluorescent plates. The devices consist ofcapillary plates and fine phosphor grains [2]. Herein, we
introduce the adding neutron sensitivity to the fine fluorescent plates for neutron imaging device.

We have developed the micro-structured fluorescentplates successfully. Impregnation with 10B-enriched orthoboric acid is effective to add neutron sensitivity to thefluorescent plates. The fabricated fluorescent plates are
expected to be useful in high-spatial-resolution imaging
devices with good detection efficiency. The next step of
the work is to increase the neutron detection efficiency.
The metal coating inside the capillary walls is considered
to be a promising method.

(;3(5,0(176 The capillary plate is made fromborosilicate glass. The specifications of the plates are as
follows: plate thickness, 0.4 mm; diameter of each capillary, 25 µm; pitch of each hole, 31 µm; open area ratio,
59 %; diameter of effective area, 20 mm. The phosphor
grains were sifted silver-activated zinc sulfide (ZnS:Ag)
with a mean particle size of approximately 7 µm [1, 2].
The plates are impregnated with 10B-enriched orthoboric
acid to add neutron detection sensitivity. The method of
impregnation is shown in )ig. 1.

a) 20 minutes drying timeb) 1 hour drying timec) Repetition is 8 timesd) Repetition is 16 times

1) The plate is put on a petri dish.

2) 10B-enriched orthoboric 3) The capillary isacid solution is fallen in
impregnated with thedrops to the dish.
solution.

4) The plate is dried inan oven at 60 ˚C.

5) Repetition of 2) - 4) processes

Fig. 1 Schematic of the orthoboric acid impregnation
method.
The neutron imaging experiments were performed at
KUR E-2. The images were collected using a CCD camera, and the results are indicated in )ig. 2.
5(68/76 Neutron induced fluorescence is clearlyobserved, however the uniformity differs according to thedrying time. Fig.2 (a) and (b) show that 1 hour drying
times seems to be enough, but 20 minutes drying is notenough. The repetition times of impregnation
increase neutron sensitivity as shown in )ig.2 (c) and (d).

Fig. 2 Results of fluorescent plates neutron imaging.
Each plate was exposed to neutrons for 10 minutes.
Image (a) drying time is 20 minutes, (b) drying
time is 1 hour, respectively. Image (c) repetition oforthoboric acid lution is 8 times, (d) repetition is
16 times, respectively. In (c) and (d), the object isa line-pair indicator [3] .
5()(5(1&(6>@ T. Sakai et al., Nucl. Instr. and Meth. Phys. Res.
B332 (2014) 1238.
>@ T. Sakai et al., JPS Conf. Proc. 11, 020005 (2016) .
>@ R. Yasuda et al., Physics Procedia 43 (2013)
pp.196-204.



‑247‑

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&2

'LIIXVLRQ0HDVXUHPHQWVRQ1$6,&217\SH6WUXFWXUHG/LWKLXP,RQ&RQGXFWRUVE\
0HDQVRI1HXWURQ5DGLRJUDSK\6 Takai1, F. Song1, H. Chen1, K. Ota1, T. Yamamoto1,
7 Yabutsuka1, T. Yao2, D. ,to3DQG Y. Saito3
*UDGXDWH6FKRRORI(QHUJ\6FLHQFH.\RWR8QLYHUVLW\.\RWR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Heterogenous doping effect, originally observed in halide solid state electrolytes, is provento be favourable in oxide solid-state electrolytes by Onishi HWDO [1] Heterogenous doping is to disperse insulative particles in Li+ ion conductors and create spacecharge layers at the vicinity of the insulative particles,
which eventually improves the overall ionic conductivityof solid-state electrolyte [2]. Such dispersion system isreferred as composite solid-state electrolytes.
In this work, neutron radiography method is applied to
study the diffusion characteristics of LATP-4wt% LLTO
composite solid-state electrolyte. Such technique has
been a standardised method developed by our group,
which utilises the difference in cross-section between 7Li
and 6Li in neutron beam, such that the diffusion profile of
6 +Li in 7Li solid-state electrolytes can be visualised. Thismethod eventually allows calculation of diffusion coefficient '* of 6Li+ [3-6].

Fig 1 (a) Original CCD camera photograph (radiography image) and (b) intensity profiles obtained by ImageJ.

(;3(5,0(176 Precursor of 7Li1.3Al0.3Ti1.7(PO4)3
and 7Li0.348La0.55TiO3 are synthesised by solid-state reaction method. By mixing the components in ratio of 96:4
and sintering, cubic pellets of 7Li LATP-LLTO composite
are prepared. 6LiNO3 paste is applied to single side of thepellets, after which the pellets are annealed at different
temperatures (300 °C, 400 °C and 500 °C) for 150
minutes to facilitate diffusion of 6Li in 7Li electrolytes.
After cooling to room temperature, the pellets are subjected to direct neutron beam radiation at B4-port in KUR.
The transmission neutron is converted to light signal by aconverter plate, which is captured by a CCD camera.
5(68/76 The original radiography image and theintensity profiles are shown in Fig. 1. By Beer-Lambert’sLaw, the natural logarithm of ,N over ,0 is proportional toFN, where ,N and ,0 are intensities of transmitted radiation
with and without scattering, FN is the light-scattering particle (in this case, 6Li+). This allows conversion of intensity profiles into diffusion profiles which are shown in
Fig. 2. It is assumed that 6Li+ diffuses down the concentration gradient, and diffusivity of 6Li+ is indifferent to its
concentration. By the semi-finite solution to the Fick’s
equation, the diffusivities of 6Li+ at different temperatures
can be calculated, which are also shown in Fig. 2. It isevident that after annealing at 500 °C for 150 minutes,
the 6Li+ is homogenised across the entire 7Li composite
solid-state electrolyte.

Fig 2 Diffusion profiles and calculated diffusivity of6 +Li .
5()(5(1&(6>@ H. Onishi HWDO. (OHFWURFKHPLVWU\.  (2016) 967.
>@ C. C Liang. -(OHFWURFKHPLFDO6RF.  (1973) 1289.
>@ S. Takai HWDO. 6ROLG6WDWH,RQLFV  (2014) 93.
>@ S. Takai HWDO. 6ROLG6WDWH,RQLFV  (2005) 2227.
>@ S. Takai HWDO. 6ROLG6WDWH,RQLFV  (2004) 107.
>@ S. Takai, HWDO. 6ROLG6WDWH,RQLFV  (1999) 165.

31130

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&2

Study on the non-destructive nuclide assay for nuclear materials with aself-indication method

J. Hori1, T. Sano2, Y. Takahashi1, and H. Yashima1

the sample and additional In filter of 0.5 mm in thickness
as a self-indicator (sample with filter run).Each measurement time was about 10 hours.

1

Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Atomic Energy Research Institute, Kindai University
INTRODUCTION: For decommissioning of Fukushima
Daiichi Nuclear Power Plants, the identification andquantification of the nuclear material in fuel debris areimportant issues for appropriate nuclear material management. However, it is considered that fuel debris contains unknown amounts of minor actinides, fission products and neutron absorbers except for nuclear materials.
Therefore, it is difficult to apply a conventional
non-destructive assay to fuel debris. Neutron ResonanceDensitometry (NRD) is one of the candidate techniquesof non-destructive nuclide assay applicable to quantity
nuclear materials in fuel debris. Especially, a
self-indication method [1] is considered as a suitable
technique for the identification and quantification of nuclides in fuel debris.
In the self-indication method, an indicator consisting of
the target nuclide is placed at the neutron beam downstream from a sample. The self-indicator is a transmission neuron detector that has high efficiency around theobjective neutron resonance energies of the target nuclide,
enabling us to quantify effectively the amount of resonance absorption of the target nuclide.
In this study, we considered the possibility of nuclear
discrimination imaging using a stationary neutron source
as an application of the self-indication method. By inserting the self-indicator filter into the beam line, thetransmitted neutrons around the objective neutron resonance energies are decreased especially. Therefore, we
expect to identify the neutron absorption due to the target
nuclide resonance without using a time-of-flight (TOF)
information.
EXPERIMENTS: The experiment was performed atthe 46-MeV electron linear accelerator in Institute forIntegral Radiation and Nuclear Science, Kyoto University.
The linac was operated with a repetition rate of 50 Hz, apulse width of 4 Ps, a peak current of about 0.5 A, and anelectron energy of about 30 MeV. The pulsed neutron
beam was collimated to 50 mm in diameter. Three foils of
In, Ag and Ta were placed in the center of beam line at a
distance of 12 m from the neutron source as shown in Fig.
1. A GEM detector (THIN-GEM, Bee Beans Technologies Co., Ltd.) was used as a neutron position sensitive
detector. The detector can obtain the two-dimensional
information of TOF for transmitted neutrons. A Cd sheetof 0.5 mm in thickness was inserted into the TOF neutron
beam line to shield thermal neutrons. Runs with andwithout the sample (sample run and blank run) were carried out. Moreover, we performed the measurement with

Fig.1 Sample arrangement of In, Ag, Ta foils for thepresent neutron imaging experiment
RESULTS: Figure 2 shows the transmission neutron
radiographs of the test sample illustrated in Fig. 1. The
spatial distribution of the transmitted neutron flux was
obtained by gating on the TOF region corresponding to
the 1.46-eV resonance of In. The region of In was clearly
identified as shown in Fig. 2(a). On the other hands, thespatial distribution of the relative counting rate in thesample with filter run to that in the sample run was obtained as shown in Fig. 2(b). Though the contrast between In and other materials was inferior to that of theimaging gated on the resonance, the region of In can be
identified. It is noted that the radiograph was obtained
without using TOF information. It indicated that the
self-indication method can be utilized to the nuclear discrimination imaging using a stationary neutron source.

Fig.2 Neutron radiographs obtained by (a) gating on theresonance region of In and (b) using the relative counting
rate in the sample with filter run to that in the sample run.
Present study was supported by JSPS KAKENHI Grand
Number JP17K07012.
REFERENCES:[1] J. Hori HWDO, EPJ Web of Conferences, 146, 09042 (2017).

31136

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&2 7KHPHDVXUDELOLW\RISKRWRILVVLRQUHDFWLRQRIXUDQLXPLQGXFHGE\EUHPVVWUDKOXQJSKRWRQVK.W. Chin, H. Sagara, J. Hori, Y. Takahashi
7RN\R,QVWLWXWHRI7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Non-destructive assay techniquefor nuclear material is one of the most important
technical issues in the field of safeguard. A nondestructive assay using photonuclear reaction has
been considered as a promising one. Previous worksuggested new method using a mono-energy Gaussian
photon beam to measure the isotopic composition of
nuclear fuel materials without relying on their selfgenerated
neutroninformation[1].
However,
producing a Gaussian photon beam requires costly
laser Compton scattering instrument. Thus, this re-searchaims to replace the source with a blemsstrahlung
photon beam from an accelerator[2]. In this work, we
tried to perform the feasibility study on the detection ofprompt neutron produced by the photonuclear reaction in
the ura-nium sample.
(;3(5,0(176 The experiment was performed at
the KURNS-LINAC. A natural uranium sheet was used asa sample and placed in the center of beam line at a distanceof about 12 m from the photon source. A platinum
target was used as the photon source ofbremsstrahlung. The linac was operated with a pulse
repetition rate of 100 Hz. The energy of electron was
optimized to 18 MeV based on the parameter survey inthe range from 8 to 30 MeV. An organic liquid
scintillator (BC-501A) with a high perfor-manceassociated with the discrimination ability between
neutron and gamma ray was used as a neutron detector.
The detector was placed at a distance of 10 cm from thesample. The signals from the detector were taken in thepulse-shape discrimination system and the two-dimensional data of pulse height and rise time were obtained.
We carried out six kinds of measurements. Three
measure-ments were done with no sample and standard
sources (Cf-252, Cs-137) without linac operation.
The remaining measurements were done with linac
operation in the fol-lowing conditions of no sample
without shields, a natural uranium sample with a neutron
shield, and a natural ura-nium sample with neutron andgamma-ray shields. In the linac experiment,
intense gamma flush and photo-neutron from thetarget is obstructive to the measurement ofprompt neutron from the sample. Therefore, twopolyeth-ylene blocks and two lead blocks were used
as shielding materials. Moreover, the electron beam
current was re-duced from 91 PA to 2 PA to inhibit
the effect of gamma flash for every run.

with that of Cs-137. However, a few gamma-ray eventswere unfortunately observed in the ROI and those should
be taken account of background. The counting rate foreach run in the ROI is shown in Table 1. We observed asignificant difference between the run of no sample andthat of uranium sample with neutron and gamma-ray
shields. Further analysis and experiment were necessary inorder to obtain conclusive evidence of the measurability ofneutron caused by photoreaction.

Fig. 1. Different cases of natural background, 252Cf,
Cs, 18 MeV beam backg round and natural uranium

137

Table 1.
52,&DVHVNatural BG
BGbeam-18MeV
252

Cf

NU+PolyB

Statistical data of counting in ROI7RWDO
7R
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52.8
0.01895()(5(1&(6[1] R. Kimura HWDO, JNST,   ,(2017).
[2] K.W. Chin HWDO, AESJ, Univ. Ibaraki, (2019).

5(68/76 Two-dimensional data of pulse height andrise time were shown in Fig. 1 for six measurements, respectively. It is noted that the horizontal axis is rising time
whereas the vertical axis is pulse height. At first, we canidentify the region of interest (ROI is shown as the dottedbox) as neutron events by comparing the run of Cf-252

31155

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Fig. 1 Experimental setup.

Fig. 2 Variation of total thermal resistance of the systemwith heat input (4K).

Fig. 3 Variation of liquid thickness with heat input.
(ࠐ:top, ‫ڧ‬:bottom, ‫ڹ‬:horizontal average)5(68/76 Figure 2 shows the variation of total thermal resistance of the system with heat input (4K). As
shown in Fig. 2, thermal resistance decreased with increasing heat input, as reported in the previous work [1].
Figure 3 shows that liquid thickness at various positions
were almost constant regardless of heat input, whichmeans that FGHP work properly with about 20 times
higher heat flux than the previous work [2].
5()(5(1&(6>@ Mizuta, K., et al., Applied thermal management, (2016) 461-471.
>@ Mizuta, K., el al., Physics Procedia,  (2015)556-563

31161

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'HPRQVWUDWLRQH[SHULPHQWVRIDQLQQRYDWLYHPHWKRGWRGHWHFWQXFOHDUPDWHULDO

M. Komeda, Y. Toh, Y. Kitamura, T. Misawa and
K. Tanabethe present new method. Thus, we could verify the innovative nuclear material detection method through theseexperiments at KURNS. This study and experiment
would make a large impact in the field of nuclear security.
A further study would be required to confirm the effects
in various conditions, such as positional dependence of
nuclear material, and would be conducted in near future.

1XFOHDU6FLHQFHDQG(QJLQHHULQJ&HQWHU-DSDQ$WRPLF
(QHUJ\$JHQF\
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR 8QLYHUVLW\

1DWLRQDO5HVHDUFK,QVWLWXWHRI3ROLFH6FLHQFH,1752'8&7,21 $ compact and low-cost
non-destructive assay system to detect hidden
nuclear material is required in the fields of nuclear
security. We have therefore developed an innovative
nuclear material detection method by using a neutron
source of Califor-nium-252, which is capable toassemble such system [1]. In this method, a neutron
source is rotated at a speed of thousands of rpm nearby
the target. Meanwhile, it is pos-sible to detect nuclear
materials by confirming the de-formation of the timedistribution spectrum obtained by a neutron detector near
the target. The machine to rotate the neutron source isless than 60 cm in width, depth, and height. The rated
output of the motor is only 750W. We installed themachine at an experimental laboratory in the KUCA, andcarried out demonstration experiments using a neutron
source (5MBq of Cf-252) and uranium.

Neutron detector
systemUranium samples
surrounded with
polyethylene
Rotation machine
Neutron source(;3(5,0(176 Figure 1 shows the overview of apparatuses used in the experiment. A neutron source wasinstalled at the outer periphery of a disc of 32 cm diameter. The uranium sample that was surrounded with polyethylene moderator set between the rotation machine andneutron detectors. The neutron detector system consistsof 6 He-3 proportional counters, which are wrapped witha cadmium plate and a boron rubber sheet in order to detect only fission neutrons effectively. The time distribution of neutron measurement was performed by a multi-channel scaler (MCS) that is synchronized with thedisc rotation. A measurement time was 15 minutes foreach experiment.
5(68/76 Figure 2 shows an example of experimental
results of a natural uranium sample and a blank sample
under the condition that the rotation speed is 4000 rpm.
The polyethylene moderator was utilized in themeas-urements of both the uranium and blanksamples. The neutron source was closest to theuranium sample ap-proximately at 6300 micro-secondsin )igure 2. Since the neutron source, theuranium sample, the polyethylene moderator andthe neutron detector system have a com-plicatedgeometry, the dips appear before and after the
peak. When the uranium sample was used, data
after
6300
micro-seconds
(from
6300
to
approximately 9000 micro-seconds) had higher
counts compared to the blank sample. This is due tothe delay effect of the interrogation neutrons (Cf-252
neutrons). The delay effect can be ob-served only
when a sample contains a fissile material undera condition of high speed rotation of Cf-252. We
could detect nuclear material for the first time by
using

Disc part where aneutron source is
attached.
Fig. 1. Overview of experimental devicesFig. 2 Experimental examples of the uranium sample(red line) and blank sample (blue line). The measurement time was 15 minutes with the rotation speed of4000 rpm.

5()(5(1&(6[1] M. Komeda, Y. Toh, Annals of Nuclear Energy,  106993.

CA3108‑253‑

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‑254‑

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T. Kobayashi, T. Sasaki, T. Saito1, K. Takamiya1, S.
Sekimoto1, M. Moniruzzaman, T. Fushimi, K. Haruki,
and T. Suzuki

acidified with 0.1 M nitric acid prior to the concentration
measurements by inductively coupled plasma mass
spectrometry (ICP-MS). The detection limit of Zr(IV) solubility was approximately 10í8.5 M.

,1752'8&7,21  Tetravalent zirconium, Zr(IV), is
known to undergo extensive hydrolysis in aqueous solution and its solubility is limited by a sparingly soluble
amorphous hydroxide solid phase, Zr(OH)4(am), in neutral
to alkaline pH range. In the presence of suitable inorganicor organic ligands, Zr(IV) solubility is increased by theformation of soluble complexes. Enhanced Zr(IV) solubility is an issue in the environmental context of safe radioactive waste disposal, because the long half-life fission
product 93Zr (T1/2=1.53×106 y) in radioactive waste forms
Zr(IV) and can migrate with groundwater under the disposal conditions. Although a very few inorganic or organic
ligands can compete with the strong hydrolysis reactions
that occur in neutral to alkaline solutions, we have foundthat several poly(hydroxy)carboxylic acids formed stablecomplexes with Zr(IV) in neutral to alkaline solutions[1].
In the present study, we investigated the solubility ofZr(IV) in the presence of three simple hydroxycarboxylic
acids (hydroxyacetic (glycolic, O20) and 3-hydroxypropionic (O21) to clarify the role of the hydroxy groups in Zr
complexation. The Zr(IV) solubility dependence on hydrogen ion concentrations (pHc) and hydroxycarboxylic acidconcentrations ([L]tot) was examined to identify the dominant soluble species and to determine their formation constants.
(;3(5,0(176 Sample solutions were prepared byan undersaturation approach. An aliquot of Zr(OH)4(am)stock suspension was added to sample solutions at selected
pHc and [L]tot (L = O20 and O21, see Fig. 1) values within
the pHc range of 7 to 13 and [L]tot range of 10í4 to 10í1 M.
Sample solutions in polypropylene tubes were kept in the
Ar-filled glove box and in some cases manually shaken fora few minutes. After given aging periods, the pHc of thesample solutions was measured and a 0.5-mL aliquot of
the supernatant was passed through an ultrafiltration membrane (3kDa, pore size a2 nm). The filtrate was5(68/76 Figure 2 shows the Zr(IV) solubility in thepresence of 0.01 M and 0.1 M glycolic acid (O20) as afunction of pHc, together with those in the absence of O20[3,4].The solubility in the presence of 0.1 M O20 equaled
10í7 M throughout the whole pHc range, and the solubility
was about one order of magnitude higher than that in theabsence of O20. Zr(IV)-O20 complexes were considered
to be the predominant Zr(IV) species in 0.1 M O20 solution. Assuming that the solid phase retained its
Zr(OH)4(am) stoichiometry, the zero slope of the log [Zr]versus pHc plot indicated that the soluble Zr(IV)-O20
complex contained four OH groups in its chemical formula.
Since the solubility increased monotonically with a slopeof two at constant pHc levels, we assumed that
Zr(OH)4(O20)22í was the major species in the solution.
 On the other hand, the Zr(IV) solubility in the presenceof 0.01 M and 0.1 M 3-hydroxypropionic acid (O21)
showed no significant increase from those in the absenceof O21. This result suggested that complexation by O21
was not strong enough to solubilize Zr(IV) under the present experimental conditions. Zr(IV) chelation featuring 5membered rings with O20 might be more stable than thatwith 6-membered rings with O21.
-2
-3
-4

log [Zr]*UDGXDWH6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\-5log [O20]tot
–2.0
–1.0

log [O21]tot
–2.0
–1.0

Zr(OH)4(am)Reference [3]Reference [4]Zr(OH)4(am)Reference [3]Reference [4]

-6
-7
-8
-9
-10
7

8

9

10

pHc

11

12

13 7

8

9

10

11

12

13

pHc

Fig. 2. Zr(IV) solubility in the presence of 0.01 M and
0.1 M O20 (left) and O21(right).

OH

O

OH

Hydroxyacetic(Glycolic) acid;
O20
S.a = 3.83 [2]OOH

3-hydroxypropionic acid;
O21
S.a = 4.61 [2]Fig. 1. Hydroxycarboxylic acids used in this study.

5()(5(1&(6[1] T. Kobayashi HW DO, J. Chem. Thermodynamics, (2019) 151-158.
[2] R. M. Smith, NIST Critically Selected Stability Constants of Metal Complexes Database Version 5.0,
Gaithersburg, USA (1998).
[3] T. Sasaki HWDO, Radiochim. Acta, 94 (2009) 489-494.
[4] M. Altmaier HWDO, Radiochim. Acta, 96 (2008) 541550.

31023

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/L&O.&O (XWHFWLF0HOWVY.Sakamura, T. Murakami, K. Uozumi, M. Iizuka andK.
Takamiya&HQWUDO5HVHDUFK,QVWLWXWHRI(OHFWULF3RZHU,QGXVWU\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
Electrorefining in molten
LiCl-KCl eutectic-based salts is the key separation process in the pyrochemical treatment of spent nuclear fuels[1,2]. It has been reported that Al cathode is suitable forcollecting actinides in the form of intermetallic compounds with a high separation factor against rare-earth
fission products [2]. Then, a chlorination process for theactinide-Al alloys using Cl2 or HCl has been examined toseparate volatile AlCl3 from actinide chlorides [3,4]. A
chemical reduction is subsequently conducted to obtainactinide metals [4].
We propose an electrorefining process to separate actinides from Al. Since U and Al simultaneously dissolve
into LiCl-KCl eutectic melts during anodic dissolution of
U-Al alloy [5], the separation between U and Al has to be
conducted at cathode. The Al-Cu and U-Cu binary phase
diagrams [6] suggest that Cu likely forms a stable alloy
with Al but not with U. In the present study, electrodeposition behaviors of Al3+ and U3+ on Cu electrode in
LiCl-KCl eutectic melts were investigated to evaluate thepossibility of electrochemical separation between U andAl.
(;3(5,0(176 A LiCl-KCl eutectic melt was contained by a high-purity Al2O3 crucible at ~723 K, where aworking electrode of Cu wire (1 mm diameter), a counterelectrode of glassy carbon rod (3 mm diameter), a
Ag/AgCl reference electrode and a type-K thermocouple
were placed. The Ag/AgCl electrode consisted of a Ag
wire immersed in a LiCl-KCl eutectic salt mixture with
1.0 wt% AgCl, which was contained in a closed-end Pyrex tube. The concentration of U3+ in the melt was increased by adding a prepared LiCl-KCl-UCl3 salt whose
U concentration was 11.4 wt% determined by ICP-AES
analysis. KAlCl4 (99.9% purity) obtained from APL Engineered Materials was used as a source of Al3+ ions because AlCl3 is highly volatile. All the experiments using
chlorides were conducted in a high-purity Ar atmosphereglove box (H2O, O2 < 1 ppm).
5(68/76 Figure 1 shows cyclic voltammograms(CVs) on Cu electrode in LiCl-KCl-UCl3 andLiCl-KCl-KAlCl4 melts. The CV in the LiCl-KCl-UCl3
melt has a cathodic current peak at -1.46 V, which corresponds to the deposition of U metal. The sharp anodic
current peak at -1.35 V is due to the dissolution of thedeposited U metal. The redox potential of U3+/U is inagreement with that previously reported [7]. There is noother distinct current peak, indicating that Cu forms

hardly any alloys with U, which was verified in the temperature range 723-823 K.
The CV in the LiCl-KCl-KAlCl4 melt has two distinct
anodic peaks at -0.75 and -0.93 V, which are due to thedissolution of Al from Cu-Al alloy and Al metal, respectively. The cathodic peak at -0.90 V, corresponding to theanodic peak at -0.75 V, is due to the formation of Al-Cu
alloy. The deposition of Al metal occurs at about -1.0 V[5]. The anodic peak at -0.65 V might be due to the Al
dissolution from different Al-Cu alloys with less Al activity. The anodic current increasing at -0.40 V is due to thedissolution of Cu into the melt in the form of Cu+ ions.
&21&/86,216
The results of electrochemicalmeasurements show that the difference in deposition potential on Cu between Al and U is 0.58 V, suggesting that
Al is expected to be highly separated from U by using Cu
as the cathode. Al electrodeposition tests in LiCl-KCl
melts containing both Al3+ and U3+ will be conducted in
the near future. The formation rate of Al-Cu alloy should
be examined in detail, which may be affected by the operation temperature. The separation technique between U
and Al investigated in this study can be applied to thetreatment of irradiated U-Al alloy fuels.
40
40

UCl3
KAlCl430
30

Current (mA)

&2

20
20
10
10
00

U metaldeposition-10-10
0.58 V-20-20-1.8-1.8 -1.6-1.6 -1.4-1.4 -1.2-1.2 -1.0-1Al-Cu alloy
formation-0.8-0.8 -0.6-0.6 -0.4-0.4 -0.2-0.2

Potential (V vs Ag/AgCl)

Fig. 1. Cyclic voltammograms obtained on Cu working electrode in LiCl-KCl-UCl3 (0.16 mol% U) and
LiCl-KCl-KAlCl4 (0.099 mol% Al) melts at ~723 K.
Scan rate 0.1 V/s.
5()(5(1&(6>@ T. Murakami HW DO, J. Nucl. Sci. Technol,  (2018)1291.
>@ P. Soucek HWDO, J. Nucl. Mater.,  (2019) 151743.
>@ P. Soucek HWDO, J. Nucl. Mater.,  (2014) 38.
>@ R. Meier HWDO, J. Nucl. Mater.,  (2018) 213.
>@ Y. Sakamura HWDO, KURRI Progress Report 2012, pp.
100.
>@ T. B. Massalski, %LQDU\$OOR\3KDVH'LDJUDPV, Vol. 1,
American Society for Metals, Metals Park, OH, 1986.
>@ Y. Sakamura HWDO, J. Nucl. Mater.,  (2018) 270.

31035

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&2

6WUXFWXUDO&KDQJHRI%RURVLOLFDWH*ODVVE\%RURQ,VRWRSH&RPSRVLWLRQ

T. Nagai, Y. Okamoto, D. Akiyama1, A. Uehara2, T. Fujii3,and S. Sekimoto4-DSDQ$WRPLF(QHUJ\$JHQF\ -$($ ,QVWLWXWHRI0XOWLGLVFLSOLQDU\5HVHDUFKIRU$GYDQFHG
0DWHULDOV ,05$0 7RKRNX8QLYHUVLW\
1DWLRQDO,QVWLWXWHRI4XDQWXPDQG5DGLRORJLFDO6FLHQFH
DQG7HFKQRORJ\ 467 *UDGXDWHVFKRRORI(QJLQHHULQJ2VDND8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 A high-level radioactive liquid
waste from a reprocessing process for spent nuclear fuelsis processed into a solidified waste made of a borosilicate
glass. We estimated the Si-O bridging structure of neutron irradiated borosilicate glass by using Raman spectrometry, and confirmed that the Si-O non-bridging
structure increased by the irradiation in our previous
study [1]. The structural change by irradiation is regarded
as the nuclear reaction 10% QĮ 7Li studied by S. Peuget,
et al [2], but the influence to a Si-O bridging structure by
the boron isotope effect has not been clear.
In this study, to understand the influence of glass
structural change by neutron irradiation and boron isotope composition, glass samples were made from enrichment boric acid reagents and neutron irradiation of
those samples was carried out in Pn-2 of KUR. The
structural change of glass sample after the irradiation will
be investigated in 2020FY.
(;3(5,0(176 Three kinds of borosilicate glass of
17B2O3-65SiO2-17Na2O-CeO2-Nd2O3-Y2O3 were prepared from raw material reagents of SiO2, Na2CO3, CeO2,
Nd2O3, Y2O3, and natural boric acid of H3BO3, enrichment boric acid of H310BO3 or H311BO3. These reagentswere loaded in an alumina crucible and were melted at
1,150°C in an electric furnace. After the molten glass
samples were solidified by cooling to room temperature,they were cut into thin plates. In this report, it is marked
with 10B-glass, natural-B-glass and 11B-glass by kind of
used isotopic boric acid reagents.
In Oct. of 2019, these thin plate samples were set in apolyethylene tube and were irradiated under the conditionof 1,000 kW for 5, 10, and 20 min in the Pn-2 of KUR.
After the radioactivity of the samples reduces to thebackground level, the Raman spectra of the samples will
be measured by using a Raman spectrometer, NRS-3100
of JASCO in KUR.
Before neutron irradiation test of glass samples, the
Si-O bridging structure difference by boron isotope
composition compared by using a Raman spectrometry

NBO, of the Si-O bridging structure [3]. The Raman
shifts of borosilicate glass samples appear in similar
wavenumber of 850-1,200 cm-1. The Raman peak of Q4
structure without NBO appeared in around 1,150 cm-1,
and those of Q3, Q2, and Q1 structures with the NBO
number = 1, 2, and 3 were in 1,090, 1,000, and 900 cm-1
respectively. The peaks of Q2 and Q3 structures can be
subdivided into plural by the Si-O-X connecting state,
and were divided into Q  , Q  , Q  , and Q  .
When the Raman shifts of 10B-glass and 11B-glass
samples were compared, the difference was observed andthe measured spectra were separated into six Gaussian
waves as shown in Fig. 1. The Raman peaks of Q1, Q 
and Q  structures of 10B-glass were higher than those of
11
B-glass, and those of Q  , Q3(2 and Q4 structures of10
B-glass were lower than those of 11B-glass. It was presumed that Si-O non-bridging structure in the borosilicate
glass increased with an increase of the 10B percentage.
The cause of the difference in Raman spectra by boron
isotope composition of borosilicate glass is unclear in thepresent, and an additional investigation is necessary.

Fig. 1. Raman spectra and separated Gaussian waves.
closed circles and fine lines are 10B-glass, and open
circles and dotted lines are 11B-glass.
5()(5(1&(6>@ T. Nagai, HWDO, 2018FY KURRI progress report,
30P10-7 (2019 >@ S. Peuget, HWDO Nucl. Inst. Methods in Phys. Res. B,  -28.
>@ P. McMillan, Am. Mineralogist,   -644.

5(68/76 The Raman spectrum of Si-O bridging
structure of a silicate glass were in the wavenumber of
850-1200 cm-1, and the peak positions of Raman shifts
were different from the number of non-bridging oxygen,

31038

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&2

6WXG\RQOHDFKLQJEHKDYLRURIFDUERQIURPQHXWURQLUUDGLDWHGVWDLQOHVVVWHHOR. Nakabayashi, S. Sekimoto1, T. Sasaki2, D. Sugiyama,
T. Fujita
5DGLDWLRQ6DIHW\5HVHDUFK&HQWHU1XFOHDU7HFKQRORJ\
5HVHDUFK/DERUDWRU\&HQWUDO5HVHDUFK,QVWLWXWHRI(OHF
WULF3RZHU,QGXVWU\ &5,(3, ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\*UDGXDWH6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\,1752'8&7,21  The speciation of 14C released
from low-level radioactive waste (irradiated stainlesssteel) is a key parameter in the safety assessment of theintermediate-depth disposal system in Japan. Most of theradionuclides released from the waste will sufficiently
decay in the disposal facility owing to the multibarriersystem. However, 14C may not be retained in themultibarrier system until it sufficiently decays, depending
on its chemical form. This indicates that it is necessary
for the safety assessment to determine the chemical formof 14C released from the waste under the disposal conditions (highly alkaline and low-oxygen conditions). To
develop an understanding of the mechanism of release of
14
C from irradiated stainless steels, leaching experiments
have been carried out using a non-irradiated stainless-steel powder in NaOH solutions (of approximately
pH 12) under low-oxygen conditions [1, 2]. The results
showed that the dominant chemical form of 12C is a colloidal carbon. If the chemical form of 14C released fromthe low-level waste under the disposal conditions is thecolloidal carbons, most of the 14C will be retained forsufficient time and decay in the disposal facility owing to
the effect of the filtration property of the engineered barrier (i.e., bentonite). In the safety assessment, this canlead to a reduced dose derived from 14C. It is essential tocarefully determine the chemical forms and clarify why
the colloidal carbons formed. In particular, there are few
data for the 14C species released from the irradiatedstainless steel under the disposal condition. Therefore, theobjective of this study is to identify the chemical form of
14
C released from the neutron irradiated stainless steel
under the disposal conditions with the leaching experiments.
(;3(5,0(176The type 316LN stainless-steel
powder (particle size ranges from 20 to 53 μm, Lot No.
F-1296, Sanyo Special Steel Co., Ltd., Japan was used inthis study. The powder was produced by a gas atomization process. The process essentially consists of the atomization of a stream of liquid metal by high-pressure
gas jets and nitrogen is taken into the metal as an impurity. The nitrogen content of the powder is 0.134 wt%,
which were taken from a mill test report (No.
1385180011) provided by the suppliers. The chemical
depth profile of the stainless-steel powder was obtainedby scanning Auger electron spectroscopy/microscopy.
The oxide thickness was estimated to be approximately 4

nm for the powder from half the decay of the oxygen
content. The oxide layer is mainly composed of iron,chromium and nickel, which is similar to the surface
characteristic of irradiated stainless steel generated by theoperation of nuclear power plants [3]. The atomized
powder (4 g) was packed in a quartz ampoule with 8 mm
in diameter and 60 mm in depth and sealed by heating the
top part of the ampoule in vacuo. These sealed ampoules
were wrapped with aluminum foil and inserted into analuminum capsule. Capsules containing the atomized
powder were irradiated for 10 hours at 1 MW in Hyd
facility of Kyoto University Reactor (KUR). The total
amount of irradiated sample is 48 g. The thermal neutron
flux was 1.63 × 1013 n cm-2 s-1 and the thermo neutron
capture cross section for the 14N(n,p)14C reaction was
1.81 × 10-24 cm-2.
5(68/76 In August of 2019, the samples were irradiated using Hyd facility of KUR. The samples irradiatedfor 10 hours are still cooled to allow for the decay ofhighly radioactive, short-lived nuclides. The 14C inventory of irradiated sample was evaluated to be very low (~2.5 × 103 Bq g-1). The corrosion rate of this sample has
not yet been clear. However, the corrosion rate of the type
316L stainless-steel powder, which is very similar tochemical composition of the type 316LN stainless-steel
powder, in alkaline condition is extremely low (~ 1.5 ×
10-13 m y-1), according to previous studies [4]. Based on
the above, the amount of 14C species released from theirradiated steel during the leaching experiment is expected to be quite low and conventional radioanalyticaltechniques for 14C detection (e.g. liquid scintillation
counting) cannot detect the 14C species in the leachingexperiment. Therefore, a high-sensitivity analysis isplanned to be carried out using accelerator mass spectrometry (AMS). AMS has a much lower detection limit
than radioanalytical techniques because AMS does notdepend on the disintegration of the radionuclide [5]. We
plan to transfer the cooled samples to CRIEPI in order tocarry out long-term leaching experiments in NaOH solutions under low-oxygen conditions. After the leachingexperiments, we also plan to quantify the chemical species of 14C in liquid and gas phases using AES.
5()(5(1&(6>@ R. Nakabayashi and T. Fujita, MRS advances, (2017) 597-602.
>@ R. Nakabayashi and T. Fujita, Radiocarbon, (2018)
1691-1710.
>@ D. Bradbury HWDO., Proceedings of International Joint
Topical Meeting of the American Nuclear Society-Canadian Nuclear Association on the Decontamination of Nuclear Facilities. (1982).
>@ R. Nakabayashi and T. Fujita, Migration 2019, (2019)
PA1-6.
>@ B. Z. Cvetković HWDO., Radiocarbon,  (2018)
1711-1727

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Solvent extraction of selenium in the nitric acid solution with selected elements

T. Kawakami, Y. Yoneda, S. Ogawa, C. Kato, S. Fukutani1, T. Matsumura2, Y. Tsubata2, K. Morita2, A. Uehara3,
and T. Fujii
Graduate School of Engineering, Osaka University
1
Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Nuclear Science and Engineering Center, Japan Atomic
Energy Agency
3
National Institutes for Quantum and Radiological Science and Technology
INTRODUCTION: As a method to preserve high level waste from spent nuclear fuel, vitrification followed bygeological deposition is considered. High level waste
contains long-lived fission products (LLFP), with somethat have a half-life of over 1,000,000 years. 79Se is a
LLFP with a half-life of 326,000 years and compared toother LLFP and minor actinides (MA), its toxicity appears earlier. Due to the half-life of 79Se, it does not poseas an immediate risk, but considering geological deposition, it would be beneficial to separate and transmutate Se
before the disposal. Selenium is also a rare earth element,
and is used for glass manufacturing and Li-Se batteries.
The separation and conversion method to reduce thelong-term toxicity of LLFP is considered in previous
studies using novel extractants [1]. However, the solvent
extraction behavior of Se is not well known with these
extractants. In this study, we focused on the separation of
Se and the solvent extraction characteristics in a nitricacid system using novel extractants proposed for the
SELECT process to understand the behavior of Se in theseparation process of MA. Furthermore, we used extractants that are known to extract Se separately [2], andtest whether it is possible to achieve high distribution
ratios with co-existence of other elements simulating thehigh-level radioactive waste solution.
EXPERIMENTS: For the organic phase, N, N, N', N',
N'', N''-hexaoctylnitrilotriacetamide (HONTA), alkyl diamide
amine(ADAAM),
N,
N,
N',
N'-tetradodecyl-diglycol amide (TDdDGA), N-phenyl
ethylenediamine (N-PDA), o-phenylenediamine (o-PDA),
and 4,5-dimethyl-1,2-phenylenediamine (DMePDA)
were used as extractants and n-dodecane, 1-octanol andnitrobenzene were used as solvents. Tetravalent Se wasdissolved in HNO3 for the aqueous phase. For the simulation of high-level radioactive liquid waste, La was selected as a representative element of light lanthanides, Dy
as a representative of heavy lanthanides, and Gd due tohaving an intermediate mass. In addition, Pd as a platinum group element in fission products, and Sr and Cs,
which are elements with a large abundance in the liquid
waste. The concentration of each element in the simulated solution are as follows: Se 1 mM, Pd 10 mM, Cs 15
mM, Sr 2.5 mM, Gd 1 mM, La 10 mM, Dy 1 mM. Bothphases were stirred for 30 minutes to perform fore extraction, and then separated by centrifugation at 2000 rpm
for 5 mins. Thereafter, HNO3 was added to the separatedorganic phase to perform back extraction. All experiments were carried out at 298 K. The Se concentration of
the aqueous phase after both extractions were measured
by Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES) and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS), and the distribution
ratios were determined.
RESULTS: The distribution ratio of Se between HNO3
and the organic phases of HONTA, ADAAM and
TDdDGA was well below 1. Using o-PDA as the extractant with octanol, and high concentration HNO3 forback extraction had the highest distribution ratio (D =3.6). Using this condition, the distribution behavior of Se
with multiple elements was observed (Fig 1). In the low
nitric acid concentration, it was D > 10 for Se, and theseparation factor for each element exceeded 1000.
CONCLUSION: Se was not extracted by the novel
extractants and remained in the residual solution. For thesimple extraction of Se, it was effective to use o-PDA as
the extractant, octanol as the solution, and concentrated
nitric acid for back extraction. Se was effectively separated from other elements in the simulated solution at low
HNO3 concentration.

Fig. 1. Dependence of D on nitric acid concentration for selected elements using o-PDA.
REFERENCES:[1] Y. Ban et al., Solvent Extr. Ion Exch., 37 (2019)27-37.
[2] Y. Sasaki et al., Solvent Extr. Res. Dev. Jpn., 24(2017) 113-122.

31062

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0RQRDPLGH5HVLQ1)DFXOW\RI6FLHQFHDQG(QJLQHHULQJ.LQGDL8QLYHUVLW\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\

2(;3(5,0(176 VBPR was synthesized by reacting
2-pyrrolidone with copolymer beads of chloromethylstyrene and divinylbenzene by following the literature[5].
Ȗ-Ray irradiation to VBPR was carried out using 6 M
HNO3 similarly to the earlier study (max. 0.2 MGy)[1].
The irradiated VBPR was separated from the supernatantliquid and washed using distilled water to avoid further
degradation by HNO3. Adsorptivities of the irradiated
VBPR to metal ions at equilibrium were obtained by abatch method. Samples of the conditioned resin (wet0.15 g) and 3 cm3 of 0.1 - 6 M HNO3 solutions containing 1 mM Re(VI) or Zr(IV), or tracer U(VI) were shaken
at 298K in a thermostatic shaking bath for 24 h. Aftershaking, samples of the supernatant were taken and theconcentrations of the metal ions were measured using
ICP-OES for Re and Zr, and ICP-MS for U. Adsorptivities were evaluated by the distribution ratio, .G.
5(68/76 Adsorptivities of VBPR irradiated in 0.1 M
HNO3 at various dose to the examined metal ions areshown in Fig. 1. The.G values for Re(VII) and Zr(IV)are found basically increased with increasing dose. For
U(VI), the identical tendency is found for lower dose, and.G values are found constant above 0.1 MGy. The .Gvalues for Re(VII) for VBPP were in an opposite manner

5H 9,,



=U ,9
8 9,









'RVH 0*\







,1752'8&7,21 It is of great importance to develop
resins with selectivity to uranium(VI) species in nitricacid media. As a part of this purpose, we have been
investigating the change in chemical structure and adsorptivity to metal ions of a cyclic monoamide resin.
The manner of structure change in the resins has beenfound basically identical, namely, starting from thecleavage of the monoamide ring by the addition of oxygen atom originating from HNO3, followed by the formation of chain monoamides by the continuous additionof oxygen. These compounds have multiple coordinative oxygen atoms, HJ, carboxyl groups, but the change
in the adsorptivity has been found different resulting
probably from the number of atoms in the ring[1-3].
More recently, our attention has been paid to long-chain
cyclic monoamides, and we have previously reported theresults for the resin consisting of 1-(4-vinylbenzyl)piperidin-2-one (VBPP)[4]. It has a 6-membered cyclic piperidine ring with a spacer between the functional carbonyl group and the main polymer chain. In the present
study, a newly synthesized long-chain cyclic monoamide
resin consisting of 5-membered pyrrolidone ring
(1-(4-vinylbenzyl)-pyrrolidone-2-one(VBPR)) was similarly investigated.

decreased with increasing dose[4], and the reason remains unclear.
It is known that the bond between methylene carbon
and nitrogen atom of tertiary-amine-type anion exchange
resins undergoes cleavage by heating or Ȗ-ray irradiation,
leading to decrease in adsorptivity to metal ions. The
results in Fig. 1 indicate that the reaction of the route (I)in Fig. 2 is dominant and that the route (II) is negligible
in the present irradiation experiments. In fact, very little
water-soluble organic compounds were detected by NMR
analysis.

Kd

Y. Yoshimura1, R. Hamashiro1, M. Nogami1, and N. Sato2

Fig. 1. Adsorptivity of VBPR irradiated in 6 M HNO3 atvarious dose to metal ions in HNO3
VBPR

(I)

(II)


CH2
OH



Fig.2. Expected major route of change in chemical structure of VBPR by Ȗ-ray irradiation in HNO3
5()(5(1&(6[1] N. Miyata HWDO, KURRI Progress Report 2010 (2011)258.
[2] M. Nogami HW DO, J. Radioanal. Nucl. Chem., (2013) 423-427.
[3] T. Nishida HW DO, KURRI Progress Report 2013(2014) 295.
[4] M. Nogami HW DO, KURRI Progress Report 2017(2018) 197.
[5] M. Nogami HW DO, Prog. Nucl. Energy,  (2008)
462-465.

31114

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‑261‑

3UHFLSLWDWLRQRIDONDOLQHHDUWKHOHPHQWVWRZDUGWKHFKHPLFDOVWXG\RI1REHOLXPS. Hayami, Y. Kasamatsu, K. Tonai, E. Watanabe, K.
Takamiya1 and A. Shinohara*UDGXDWH6FKRRORI6FLHQFH2VDND8QLYHUVLW\
,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Nobelium (No) with atomic number 102 is one of actinide elements. It is reported thatstable oxidation state of No is +2 although those of theother heavy actinide elements are all +3. The chemical
behavior of No is reported to be similar to that of group 2elements in HCl [1]. However, it is difficult to investigate
the chemical properties of No because of low production
rates and short half-lives of the No nuclides. Therefore, it
is important to conduct fundamental experiments ofGroup 2 elements for chemistry of No.
Previously we reported new experimental method inwhich the hydroxide complexation of the target elements
can be studied from the coprecipitation behavior withsamarium hydroxide [2]. So far, we have qualitatively
investigated the coprecipitation behaviors of various elements, and we successfully applied the method to element 104, rutherfordium (Rf). Recently, coprecipitation
experiments with group 2 elements that are comparative
elements for No have been in progress. In this study, both
coprecipitation and precipitation experiments were performed for Group 2 elements Ca, Sr, and Ba. In addition,in order to elucidate the new chemical properties of No,
we focused on the reaction with sulfate ions, and conducted experiments on coprecipitation behavior of theseelements with BaSO4 using ammonium sulfate in addition to sulfate precipitation experiments.

Sr or Ba chloride solution was added. After mixing it, 2
mL of 0.01, 0.1, or 1.0 M (NH4)2SO4 solution was added
to generate sulfate precipitate. These solutions werestirred for 5 min at room temperature. The precipitates
were collected with membrane filter by suction filtration.
The precipitate and filtrate samples were then dried onheater at 100 degree C and were assayed bu J-ray measurements. The coprecipitation yields were determinedfrom radioactivity of the J-ray measurements.
5(68/76 The precipitation (ppt) and coprecipitation(co-ppt) yields were determined from the equation: $ppt /($ppt + $fil), where $ represents the radioactivity, and ppt
and fil indicate the precipitate and filtrate, respectively.
In the hydroxide precipitation and coprecipitation experiment, the yields of precipitation of Ca, Sr, and Ba
were very low at low [OH-] and increased in high [OH-].
However, the yields of coprecipitation of Sr, and Ba werehigh at low [OH-] and almost zero at high [OH-]. These
results might be due to the facts that for alkaline earth
metal elements, formation of polynuclear precipitates andspecies were reported in macro scale. Coprecipitation
behavior is considered to relate to the behavior in amononuclear precipitate. Since the No can be dealt assingle atoms, the data on coprecipitation behavior would
be able to be used as comparative data to discuss thecomplex formation of No.
In the sulfate precipitation and coprecipitation experiments (Fig.1), it was found that the coprecipitation behavior of Sr and Ba was basically consistent with that inprecipitation. Differences were also found in the coprecipitation yields among group 2 elements which are
qualitatively consistent with their solubility products.
SSWRUFRSS\LHOGV

&2(;3(5,0(176 85Sr and 133Ba samples were prepared by irradiating protons on pellet samples of RbCl for
1 h and of CsCl for 10 h using the AVF cyclotron at
RCNP. 47Ca sample was prepared by irradiating thermal
neutrons (3×1013 cmí2 sí1) on a powder sample of CaO
for 1 h using the reactor at KUR. They were separated
from other majority of radioisotopes by cation-exchange
and anion-exchange methods.
In the hydroxide coprecipitation experiment, 20 PL (20Pg) of Sm standard solution (1 M HNO3) was added into
the 85Sr or 133Ba solution. In case of the precipitation experiment, 20-1000 g of Sr or Ba chloride or 10 mg of47
CaO in aqueous solution was added. After mixing it, 2
mL of basic solution was added to generate hydroxide
precipitate. In the present experiment, we used dilute orconcentrated NH3 solution, or 0.1, 1, or 6 M NaOH solution as the basic solution to observe the dependence ofthe precipitation yield on the concentration of the basic
solution.
In the sulfate coprecipitation experiment, 20 L (20g) of BaCl2 solution was added to the 85Sr or 133Ba solution. In case of precipitation experiment, 20-1000 g of

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Fig. 1. The yields in sulfate precipitation and coprecipitation experiments.
5()(5(1&(6[1] R. J. Silva HW DO., J. Inorg. Chem., , 9, 2233-2237(1974).
[2] Y. Kasamatsu, HWDO., Appl. Radiat. Isot. , 105-116(2016).

31153

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&2

Effective Measures on Safety, Security, Hygiene and Disaster
Prevention in Laboratories

T. Iimoto, Y. Igarashi, J. Nakayama, R. Miura,
K. YamamotoDQG T. Takahashi

of small amount of U and Th” and “radiation educationand human resource development in secondary schoolfrom global viewpoint” through our member discussion.

The University of Tokyo,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\INTRODUCTION: Important aspects of the study canbe found in the following keywords, such as safety, security, hygiene and disaster prevention. Nuclear
research reactor is one of representative facilities
together with these keywords under their operation. It
is effective to investigate the latest status on practicalmeasures on these keywords in various facilities
including nuclear research reactors, to compare eachother among facilities, and to discuss more optimized
ones for our positive safety management. Throughthis process, it is also essential to investigate the latest
international and/or national regula-tions and the
movement of revision of them. In addition, developmentof human resource and public literacy on nuclear
science and technology is also within the scope of theresearch. The total discussion contents and their fruits are
directly useful for all relating laboratories.
RESEARCH APPROACH:
General research approach is as follows.
- Measures of safety management during operation or
standstill status of the real facilities would be investigated. This information would be used for our research
discussion on the positive and more optimized safety
management.
- It would not be a single year research, but maybe two to
three years research for one theme.
- Information source of facilities would not be only KUR,
KUCA or the other facilities in Kyoto University, butalso the Kinki university research nuclear reactor or thefacility of National Institute of Fusion Science, etc. This
research is an active joint-research with these relating
facilities and positive researchers on safety management.
- One of the distinctive features of this research is to involve office staffs as cooperators as well as researchers
and technical staffs. In The University of Tokyo, most of
the members in Division for Environment, Health and
Safety are office staffs who knows real situation ofsafety management in laboratories very well.

Concrete discussion target in FY of 2019 was determined
as following two; “standardizing education system forsafety managers and users in universities for application

EDUCATION SYTEM IN UNIV. FOR SMALLAMOUNT U&Th APPLICATION:
Safety education system for managers and users of small
amounts of U and Th has been discussed to standardize itin universities. Latest status of their education in several
Japanese universities have been investigated and concluded the common and needed viewpoints. In addition,
throughout this discussion, not only good practices andideas for nuclear material safety management at the laboratory and laboratory levels, but also issues to be
overcome under the current Japanese legal system wereshared. The discussion fruits are started to be opened
through technical journals, for example, the first article
was published in the early 2020 as the reference [1].
RADIATION EDUCATION AND HRD IN SECONDARY SCHOOL:
International
AtomicEnergyAgency(IAEA)RAS0065/0079 (2012-2021) Technical Cooperation Programme (TCP) relating secondary school education on
nuclear science and technology (NS&T) in Asia and Pacific region became a trigger for us to organize TeamJAPAN. This team consists of several Japanese experts to
support the activities and develop several educational
tools and modules with “WOW factor” using the
STREAM (Science, Technology, Robotics, Engineering,
Arts and Mathematics) education concept. So far, a
hand-made Air-GM counter, a wide-view Peltier typecloud chamber, a handy radiation monitor for school application, motivation-up movies, etc, has been developedby us. Team JAPAN continues its activities with the cooperation with experts, teachers, and other stakeholders
in the world. The discussion fruits are started to beopened through technical journals, for example, several
articles were published as the reference [2][3][4].
REFERENCES:>@ K. Yasuda, M. Yasuda, T.Iimoto et.al., RADIOISOTOPES, 69 (2020)
>@ T. Iimoto et.al., Journal of Radiation Emergency
Medicine, 8 (2019)
>@ K. Katengeza, T. Iimoto et.al., Japanese Journal of
Health Physics, 54(2019)
>@ T. Toda, T. Iimoto et.al., Radiation Protection Dosimetry, 184 (2019)

31018

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&2

6FLHQWLILF(WKQRJUDSK\IRU1XFOHDU6FLHQFH3DUW5HVSRQVLELOLW\RI6FLHQFH3RVW,,WDWH9LOODJH)XNXVKLPD

M. Takagaki and S. Masunaga

recovery of wealth, will return the basic science toinvestment (positive feedback), and the position ofscience will be politico-economically jeopardized(Fig.1).

/RXLV3DVWHXU&HQWHUIRU0HGLFDO5HVHDUFK ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\In this report, we will report the ethnography of theretuned residents of Iitate Village in the 9th year
after the disaster in two parts. Part 1 is about the
responsibility of science, which is the main subjectof this research. In Part 2, I will briefly report on
the criticism of science that can be intensely drawn
from the story of villagers who lives in nature.
Former UNSCEA Commission on Radiation
Effects Prof. Wolfgang Weiss stated the
responsibility for science after the Fukushima
nuclear accident as follows; “The most serious
damage caused by Fukushima accident is thatpeople lost trust for science and scientists. Thiscertainly will influence long- term human history,
and we cannot recover such situation so easily. We
scientists are responsible to such situation.” (Prof.
Wolfgang Weiss)
Clearly explaining the responsibility of science isdifficult. Because it is an essential factor
unavoidably embedded in the uncertainty of science.
What is science to humanity? In particular,
regarding the responsibility of science in nuclear
accidents, it is important to structurally analyze
various factors in addition to science and approach
where responsibility lies. There are much factors
involved such as politics, economy, energy andenvironment are numerous. There is always adanger in using the results of natural science as atechnology in society. Technology is always
absorbed by human society while maintaining a
sympathetic relationship with safety, such as danger
due to immaturity of technology and danger as thesum total due to interaction with other technologies.
Nuclear power generation technology has been used
for human welfare while balancing danger andsafety issues at unrealizable levels.
Occasionally, in the human society, it is notuncommon for security to be neglected by paying
attention to the return of capital based on the logic
of investment.Once the basic science is put into
practical use and used as a technology in society(politico-economic engine), the logic of capital,such as investment in technology and recovery and



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Fig.1 Politico-economic engine for technologizing
the science.
Scientists should be discreet enough to apply theirscience findings to technology. If the principle ofcapital intervenes at this stage, science will possibly
become a non-science, and it will become one of
the engines absorbed by the capital principle astechnology, and the location of risk will no longer
be clear. Professor Hideki Yukawa, who was thefirst member of the Reactor Promotion Committee
under the Nakasone administration, resigned in
opposition to the promotion of nuclear technology,
saying that safety could not be guaranteed. I don't
know if his actions can be justified, but it could beconsidered as a waiver of scientists' responsibility. I
have long argued for the need for regulatory
anthropology, but few researchers have shown
understanding. A cultural anthropology departmentthat investigate the safety of nuclear science withthe peace of mind that the public is convincedshould be installed in a nuclear research institute.
Is it possible to regulate so that both scientificsafety and psychological security can be achieved at
the same time, or not? Such regulation science does
not exist in much fields of our natural science, butrather in fields of medicine and drug safety.
Approximately 10 years before the accident
occurred, National Institute of Radiological
Sciences (NIRS) tried to advance the field of
regulatory science, but the Science and Technology
Agency at that time showed little understanding. It
means that the Science and Technology Agency
was just for promoting nuclear power, so safety wasjust an excuse. I wonder if the gaps around it will
be filled up a little with anthropology.

&2 $VVHVVPHQW RI QRQKRPRJHQRXV H[SRVXUH RI UDGLDWLRQ ZRUNHUV LQ DFFHOHUDWRU IDFLOLW\± VLWXDWLRQLQWKHVPDOOOLQDFIDFLOLW\around 100 μSv h-1. The physical phantom with the OSL
dosimeters was set for 18 hours and the OSL dosimeters
were read after the irradiation.

M. KRZDWDUL and T. KXERWD
&HQWHUIRU$GYDQFHG5DGLDWLRQ(PHUJHQF\0HGLFLQH
1DWLRQDO,QVWLWXWHVIRU4XDQWXPDQG5DGLRORJLFDO6FL
HQFHDQG7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
.\RWR8QLYHUVLW\,1752'8&7,21  The reduced occupational dose
limit for the lens of the eye has been adopted by the International Atomic Energy Agency [1], the European
Union [2] and the United States [3]. Annual equivalentdose limit for the lens of the eye for occupational exposure in planned situations was reduced from 150 mSv to
20 mSv averaged over five consecutive years and 50 mSv
in any single year. Comprehensive survey was madeand the technical document for eye lens monitoring has
been released from the IAEA [5].
The study focuses on how the inhomogeneous exposureof radiation workers due to radiation from activated apparatus of the accelerators can be assessed. The purposeof the study is to evaluate whether the additional monitoring of the eye lens dose is required for the radiation
workers in the accelerator facility. The authors introduce
a quantitative index, HI which expresses how much radiation workers are exposed non-homogeneously for theirradiation work. HIs were defined as the ratio of the personal dose equivalent for the eye lens and the extremity
monitoring to that for the whole-body monitoring.
(;3(5,0(176 We focused on the exposure situationof radiation workers who are engaged in the handling of
the activated target in the linac facility. The HIs for thisexposure situations were experimentally evaluated usingawater-filledphantomwiththeOptically
Stimulated
Luminescence(OSL)
dosimeters(nanoDotTM, Nagase Landauer Ltd.) incorporated with awater-filled phantom. The phantom was placed in theworkplace to mimic the respective work Since
inhomogeneous exposure will be expected in terms ofextremities as well as the lens of the eye, OSL
dosimeters were put on the fingers and palms of thephysical phantom. The ambient dose equivalent rateof the vicinity of the target was measured to be5(68/76 Table 1 was listed the comparison of theratio of the eye lens dose or the extremity dose to thetrunk dose measured on the physical phantom set close to
the accelerator target for mimicking the target handlingand adjustment. Table 1 also showed the results of theratio of HIs analytically estimated in accordance with theinverse square law of the radiation emission. The theoretically estimated HIs can predict the measured HIs
within factor two. However, the discrepancy between
analytically estimated and measured HIs were found tobe factor 5. This might be explained by the difference ofthe exact distance between the source and the hand(palm) and the influences of the shielding and the source
shape of the target.
5()(5(1&(6[1] International Atomic Energy Agency (IAEA). Radiation protection and safety of radiation sources: International Basic Safety Standards. General Safety
Requirements Part 3.
[2] European Union (EU). Basic safety standards forprotection against the dangers arising from exposure to ionizing radiation. Council Directive
2013/59/EURATOM.
[3] NCRP Commentary No. 26 - Guidance on Radiation Dose Limits for the Lens of the Eye (2016).
ISBN 978-0-913392-17-1.
[4] ORAMED: Optimization of Radiation Protection of
Medical Staff, EURADOS Report 2012-02. ISBN
978-3-943701-01-2.
[5] International Atomic Energy Agency (IAEA). implications for occupational radiation protection of
the new dose limit for the lens of the eye.
IAEA-TECDOC-1731.
(2013),
ISBN
978-92-0-115213-8.

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31050

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G. Yoshida, K. Nishikawa, Y. Sakaki, Y. Morikawa1, M. gress, variations of elemental concentration in concrete ofInagaki2, S. Sekimoto2, T. Miura, A. Toyoda, H. Matsu- the samples were determined as shown in Fig. 1. The
concentration of cobalt and europium had been discussed
mura and K. Masumotoin elsewhere [4]. We will discuss the other elements inthe near future. Currently, we are working on a database
5DGLDWLRQ6FLHQFH&HQWHU.(.$FFHOHUDWRU/DERUDWRU\.(.
of accelerator facility concrete measurements and plan to,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
update it as needed.
.\RWR8QLYHUVLW\,1752'8&7,21  We are working on the researchfor establishment of more reasonable decommissioning
process of accelerator facilities with the aid of Japan
Nuclear Regulation Authority. Especially, concretematerials used as shields and buildings occupy the mostamount of weight in a facility, and significantly
contribute to the cost of decommissioning. The generated
radionuclides should be identified in advance and waste
should be separated into activated and non-activated are-asfor efficiency and waste reduction, when decommissioning an accelerator facility.
However, the assessment of an activation concrete material is not easy. Currently, the destructive analysis by core
boring is the only method of investigating that. From thisbackground, we had developed a breakthrough method toestimate the activity of 60Co and 152Eu in activated concrete in the accelerator facility from the contact dose ratemeasurement with a survey meter [1,2]. This methodstrongly depends on the concentrations of cobalt and europium which is trace elements in a concrete. From theviewpoint of practical use, the variation of trace elements
concentration in the concrete must be understood.
We also had developed the method for prediction theactivity in the concrete material at future, by measuring
the activities of 24Na and 56Mn immediately after theaccelerator operation [3]. For this method, information ofvariation of natural sodium and manganese in concrete ofaccelerator facilities is indispensable.
In this study, we analyzed trace element concentrations in
concrete samples of some accelerator facilities in Japan
with neutron activation analysis which suitable for traceelement analysis of ppm order, and compared the result.

Fig. 1. Variation of elemental concentration in
concrete samples of accelerator facilities determinedby neutron activation analysis.

(;3(5,0(176 Total 89 of core concrete samples
collected from 8 facilities were prepared as irradiation
samples. (DFK FRUH VDPSOH ZHUH JURXQGHG WR  ȝPmesh particle size by a ball mill. Two igneous rocks (JA-1, 5()(5(1&(6JG-3) were employed as references and prepared in the >@ H. Matsumura, A. Toyoda HWDO., J.Phys.Conf.Ser., (2018) 0120016.
same way. For analysis of short-lived nuclides generated
by neutron irradiation, 40 samples were irradi-ated at Pn-3 >@ H. Matsumura, G. Yoshida HWDO., Environmental
Radiochemical analysis VI, (2019) 135-147.
with 1 MW during 10 s, and measured with a Ge detector
immediately after irradiation. All samples including the >@ H. Matsumura, G. Yoshida HWDO., Radiation
Protection, in Press
above 40 samples were irradiated at Pn-2 with 5 MW>@G.
Yoshida, K. Nishikawa HWDO., J.Radioanal.
during 3000 s, and measured with a Ge de-tector after short
Nucl.Chem.
in Press
lived nuclides were attenuated.
5(68/76 From the gamma-ray spectra of the samples, total 26 radionuclides generated by neutron capture
reaction were identified. Although the analysis is in pro-

31056

‑266‑

&2 &RPSDULVRQRI&KORULQH&RQFHQWUDWLRQLQ(DFK0XQLFLSDO6ROLG:DVWH)UDFWLRQ0HDVXUHG
E\1HXWURQ$FWLYDWLRQ$QDO\VLVDQG%RPE&DORULPHWHU,RQ&KURPDWRJUDSK\
K.. 2Vhita, S. Hayasaki, S. Fukutani and M. Takaoka'HSDUWPHQWRI(QYLURQPHQWDO(QJLQHHULQJ*UDGXDWH
6FKRRORI(QJLQHHULQJ.\RWR8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 In recent years, plastic contained inwaste has become a serious problem worldwide. Specifically, from the viewpoint of hazardous substances, someplastics generate hydrogen chloride and organic chlorinecompounds when they burn, so information on chlorine isnecessary. Therefore, in this study, the chlorine in eachfraction contained in the municipal solid waste (MSW)
was analyzed by the bomb calorimeter - ion chromatographic method (B-IC) and the neutron activation analysis (NAA), and the results were discussed and compared.

concentration. In particular, wrapping plastics exceeded
300,000 mg/kg by either method. It is conceivable thatthe chlorine content of the plastic as a whole and of the
MSW as a whole will change greatly depending on how
much of the wrapping plastics accounts for.
The chlorine concentrations measured by the two methods were compared (Fig.1). The slope of the regression
line was 0.873, the correlation coefficient was 0.997, andthe p-value was 1.5×10-16, indicating a correlation. The
chlorine concentration measured by B-IC was smaller
than that measured by NAA, neutron activation analysis,
and it was considered that only combustible chlorine wasmeasured by the former.
Table 1 Chlorine conc. in each fraction of MSW measured by
NAA and B-IC.
Items(;3(5,0(176 The MSW sampled from the pit of the
MSW incineration facility of municipality A was classified into 20 categories, dried at 100 °C, and then homogenized to 2 mm or less with a crusher. Chlorine measurement was carried out for 16 categories listed in the
Table 1 in which sufficient amounts were obtained formeasurement. First, NAA for chlorine was performed
four times for each sample. Samples were irradiated for 5
min with a thermal neutron flux of 2.0–2.4×10 13 cm-2࣭S-1
at KURRI. 38Cl (t1/2 = 37.18 min, EȖ = 1642, 2168 keV)
were measured by using a Ge semiconductor detector for
60 sec. Chlorine conc. was also measured once by B-IC
based on JIS K 7302-6 [1]. 

Kitchen wastes

PapersTextilesWaste wood and grass

Plastics

OthersLeft untouched or uncooked foods
Others kitchen wastes
Disposable diaper for adults
Disposable diaper for infants
Used papers (Newspaper, Magazine, etc.)
Packing papers (Cardboard, Carton)
Other papers
TextilesWaste wood and grass
Packing plastics
PET bottles
Plastic container for lunch pack
Other plastics
Wrapping plastics
Rubber and leather
Others (Combstibles)

NAA
mg/kg
10,1008,210
6,170
13,30011,400
2,480
4,140
3,200
1,530
17,7001,690
10,70060,800339,000
142,000
8,090

B-IC
mg/kg
13,0006,120
6,180
18,000
1,360
1,100
2,030
1,130
729
8,510
913
7,880
63,000300,000
108,000
13,0001,000,000
Chlorine conc. measured by B-IC (mg/kg)

5(68/76 The chlorine concentrations measured by
NAA and B-IC are shown in the Table 1. The differencein chlorine concentrations between the two methods was
small except for used papers.
Regarding the kitchen wastes, the chlorine concentrationof other kitchen wastes was smaller than that of the left
untouched or uncooked foods. Except for the results of
NAA for used papers, the chlorine concentration of disposable diapers was higher than that of other paper fractions. Especially for disposable diapers for infants, NAA
result was about 13,000 mg/kg and B-IC result was about
18,000 mg/kg. It has been reported that it has not been
disposed so long and that urine contains 8,600 mg/L ofchlorine [2]. The high chlorine concentration in the disposable diaper is considered to be due to the adherence ofchlorine derived from human. As the amount of disposable diaper waste increases with aging society, it is expected that the chlorine concentration in all papers will
increase. The chlorine concentration of textiles, waste
wood and grass were lower than that of the other categories. Plastics, except for PET bottles, generally had a highchlorine concentration. Although the composition of PET
bottles does not contain chlorine, it is considered thatchlorine was detected due to the adhesion of beverages
and the like on the bottle. Wrapping plastics, other plastics, rubber and leather had a significantly high chlorine

Sub-Items

y = 0.8727x - 509.39
R² = 0.9931
100,000

10,000

1,000

100
100

1,000

10,000100,000

1,000,000

Chlorine conc. mesured by NAA (mg/kg)

Fig.1. Relationship of chlorine conc. measured by between
NAA and B-IC.

5()(5(1&(6[1] JIS K 7302-6, Densified refuse derived fuel í Part 6 :Test method for total chlorine contents, 1999.
[2] H. Nakanishi, Progress of night soil treatment techniques, -DSDQMRXUQDORIZDWHUSROOXWLRQUHVHDUFK, Vol.14,
No.11, pp.766-771, 1991.

31075

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Y. Igarashi, Y. Wang1, J. Nakayama2, T. Misawa3, T.
Takahashi3 and T. Iimoto2

because the radon concentration was not controlled.
Therefore, the indoor condition in which the radon concentration will increase naturally was set.

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7RN\R

1XFOHDUDQG5DGLDWLRQ)URQWLHU7HFKQRORJ\5HVHDUFK&HQWHU&KLQD,QVWLWXWHIRU5DGLDWLRQ3URWHFWLRQ'LYLVLRQIRU(QYLURQPHQW+HDOWKDQGVDIHW\7KH8QL
YHUVLW\RI7RN\R,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 This study focuses on improving a
prototype monitor for accurately and versatilely measuring the concentration of radon and its decay products in
response to increasing international demand for monitorsthat measure both radon and its decay products under
several conditions. We have already developed the prototype monitor based on the two-filter method. The measurement target of this method is α-ray from 218Po generated from the decay of 222Rn as shown in Fig.1.

5(68/76 DQG ',6&866,21 Radon concentration(Bqm-3) measured by the calibrated radon concentration
monitor and the number of counts (cpm) measured by the
prototype monitor are shown in Fig.2. From the results in
Fig.2, the radon concentration increased to about 300 Bq
in 50 hours with a tendency similar to the previous study[2]. The number of counts measured by the prototype
monitor also increased to about 15 cpm in 50 hours. On
the other hand, large fluctuations in both the concentration and the counts were observed after 45 hours. Thesebehaviors were caused by unexpected changes in themeasurement environment. Therefore, the conversion
factor of relation the concentration and the count wascalculated from the measurement result obtained from thestart to 44 hours after. As a result, an average value of theconversion factor was 17 Bqm-3 / cpm.

Fig. 1Fig
1. Radon concentration meas
measurement
rement apparat
apparatussof 2filter method.
Through simple calibration tests and characteristic testsof the prototype monitor, we selected the suitable detector position for measurement and filters for up-streamside and down-stream side. From the results of these tests,
we developed a new prototype monitor that can measureaccurate radon concentration. The conversion factor fromthe counts of prototype monitor to the radon concentration was also obtained [1]. In order to evaluate the measurement ability of the new monitor, we measured radon
concentration in the reactor room of KUCA where thefluctuation of radon concentration is close to that in thenatural environment using the monitor.
(;3(5,0(176 To measure the radon concentration
in KUCA reactor room, the new prototype monitor using
two-filter method and a calibrated radon concentration
monitor (RAD7) were installed in the room to comparewith the results of these monitors. Experimental conditions of the prototype monitor were; detector: PIPS
CAM300-17AM(40V),
Upstream-side
filter:
No.4A+HE-40T, Downstream-side filter: GF/F, distanceof detector-filter: 5mm, pump flow: 10L min-1. The
measurement interval was set to 1 run: 5 min × 5 times=
25 minutes, and this run was repeated for 50 hours. All
ventilation systems of the reactor room were stopped

Fig. 2. Radon concentration (Bqm-3) of the RAD7
and number of counts (cpm) of the prototype monitor
in KUCA reactor room.
From the above results, the radon concentration measurement for a long time can be performed stably underthe environment that a radon concentration naturally increases. There are some problems that the unintended
noise significantly affects the measurement results.
Therefore, it is necessary to consider an operating methodthat can eliminate the noise for outdoor measurements. In
the future, we will improve the prototype monitor tomeasure the deposition of particulate nuclides on the inner wall of the decay chamber and the effect of the aerosol for the radon decay products to investigate for theoperational stability of the concentration measurement ofradon decay products.
5()(5(1&(6>@ Y. Igarashi HWDO, Rad. Prot. Dosim., (2019)421.
>@ KUR Aerosol Research Group, KURRI-TR-232(1982)

&$3115‑270‑

&2,VRWRSH'LOXWLRQ1HXWURQ$FWLYDWLRQ$QDO\VLVIRU4XDQWLI\LQJ+DIQLXPT. Takatsuka, K. Hirata, Y. Iinuma1, R. Okumura1,
H. Yoshinaga, and K. Takamiya1
1DWLRQDO0HWURORJ\,QVWLWXWHRI-DSDQ1DWLRQDO,QVWLWXWH
RI$GYDQFHG,QGXVWULDO6FLHQFHDQG7HFKQRORJ\,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Hafnium (Hf) oxide is utilized as
high-N dielectric films for semiconductor devices especially with fast and low-power operation. Additionally,
the films are being introduced as ferroelectric material on
ferroelectric transistors and memories. The device fabrication process should be precisely controlled for such
dielectric films. We aimed to quantify Hf in Hf oxide
films in weight unit by means of isotope dilution-neutron
activation analysis (ID-NAA) [1].
(;3(5,0(176 Hf oxide films were deposited on
4-inch Si wafers by magnetron sputtering. The target
thickness was set to 4 nm. The prepared wafers with thefilms were cut into 10 mm × 10 mm pieces for the measurements.
The procedure for ID-NAA has two sequences of an
isotope dilution (ID) and a reverse-ID to ensure traceability to the SI units; the latter sequence was performed todetermine the Hf concentration in a spike solution byreferring to a Hf standard. The spike solution was prepared by dissolving 174Hf-enriched Hf oxide (Oak Ridge)
in a HNO3 + HF aqueous solution, and by diluting to aproper concentration. For calibrating the amounts of Hf, aworking standard solution was prepared by diluting NIST
SRM 3122 gravimetrically. For the ID analysis, small
amount of the spike solution was dropped onto each Hfoxide sample (HfO2+Sp), while the spike solution or
standard solution was dropped separately onto each pieceof cleaned filter paper (Sp or STD), as shown in Fig. 1.
For the reverse-ID analysis, the spike and standard solutions were dropped onto one piece of filter paper(Sp+STD).
For validation, the Hf concentration of the spike solution was also determined by NAA with internal standards.
Four concentration levels of working standard solutions
were prepared; an internal standard solution of Sb fromNIST SRM 3102, three Hf and Sb mixed standard solutions with different Hf concentrations for the calibration.
For the quantification of the spike solution, the specimens
were prepared using the spike solution before diluting
since the diluted spike solution has little Hf-180 to bequantified. Weighed portion of the spike solution was
dropped onto a filter paper followed by dropping the Sb
standard. As for standards, aliquots of the working standard solutions of Hf and Sb mixture were weighed anddropped onto filter papers.

Fig. 1. Sample preparation for ID-NAA.
All the samples were sealed up separately in cleanpolyethylene bags, followed by being stacked in a polyethylene container for the neutron irradiation. The irradiation was performed for 4 hours with a 5.5 × 1012 cm-2·s-1
thermal neutron fluence rate at Pn-2 in the Kyoto university research reactor (KUR). The gamma-ray activity ofeach sample was measured by a high-purity germanium
detector (CANBERRA).
5(68/76 From the gamma-ray spectrum, the gamma-ray intensity ratio of 175Hf to 181Hf and 181Hf to 124Sb
were calculated for ID and internal standard method, respectively. The Hf concentration in a spike solution wasdetermined to be 6.63 mg/kg by reverse-ID. The amountsof Hf in the Hf oxide samples were calculated from theintensity ratios based on a formula reported in Ref. 1.
Dividing the Hf amounts by measured sample surface
areas, the area densities were calculated to be
3.64 μg·cm-2 and 3.63 μg·cm-2 for two measured samples.
From the calibration curve by internal standard method in
Fig. 2, the spike concentration was determined to be 108
mg/kg. For comparison, the determined spike concentrations were converted into the relative ones to the nominal
concentrations since the nominal concentrations weredifferent from each other. The resultant relative concentrations were 0.982 and 0.978 for reverse-ID and internal
stand method, respectively. This agreement showed thereverse-ID procedure in ID-NAA was appropriate for thequantification.

Fig. 2. Calibration curve for determining the spike
concentration by the internal standard method.
5()(5(1&(6[1] C. Yonezawa HWDO, Anal. Chem.,  (1983)
2059-2062.

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&2 6WXG\RQ6XSHUSRVLWLRQRI7HUDKHUW]&RKHUHQW5DGLDWLRQ8VLQJD5LQJ5HVRQDWRU
N. SeiDQG T. Takahashi1
5HVHDUFK ,QVWLWXWH IRU 0HDVXUHPHQW DQG $QDO\WLFDO ,Q
VWUXPHQWDWLRQ 1DWLRQDO ,QVWLWXWH RI $GYDQFHG ,QGXVWULDO
6FLHQFHDQG7HFKQRORJ\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21  Research on nonlinear spectroscopy has been explored in the terahertz (THz) region
where low-energy excitations and photoinduced phasetransitions can be observed, and developments of broadband THz light sources with high peak power have been
desired [1]. A short-pulse relativistic electron beam issuitable for generating coherent radiation in the THz region, and THz light sources and their applications havebeen developed in a lot of accelerator facilities [2]. As
coherent Cherenkov radiation matched to a circular planewave, which was demonstrated in our past joint research[3], a method for extracting high-power THz light fromthe relativistic electron beam by devising a principle oflight emission has been mainly studied. Although thedevelopment of a new high-efficiency principle of lightemission was important factor for realizing high-powerTHz light, this approach alone was not enough.
Therefore, we proposed that coherent radiation generated by a pulse train of electron bunches was confined ina ring resonator and superimposed with the same phase.
We succeeded in observing THz light pulses extracted
from a ring resonator in an L-band linac at Kyoto University Institute for Integrated Radiation and Nuclear
Science (KURNS-LINAC).

passing through the collimator injected to a hole with adiameter of 5 mm on an aluminum thin foil and generated
coherent forward diffraction radiation in the ring resonator. Furthermore, the electron beam passed through analuminum thin foil and generated coherent backward
transition radiation. The current of the electron beam
passed through another aluminum thin foil was approximately 60 PA. These aluminum thin foils were also usedas mirrors constituting the ring resonator. The two coherent radiations were confined in the ring resonatorcomposed of four mirrors, which included two parabolic
mirrors with the focal length of 508 mm. The length of
the resonator was 922 mm, which was four times the interval of the electron bunches. A part of the resonant light
was extracted from the resonator through the hole formedin the aluminum thin foil and transported to an experimental room. The transported resonant light was detectedby a D-band diode detector (Millitech Inc., DXP-06), andthe output power was measured by an oscilloscope withthe frequency band less than 350 GHz.
5(68/76 Figure 2 shows a macropulse of theTHz-light power measured by the D-band diode detector.
Although the temporal resolution of the measured
THz-light power was insufficient due to the low frequency band of the oscilloscope, it was found that thedetector could identified coherent radiation generated byeach electron bunch. By using an oscilloscope with awider band, it will be possible to observe the micropulse
waveform of the resonant THz light and to adjust thelength of the resonator. We also plan to extract the THz
light from the resonator using a thin film which hardly
absorbs light in the THz region.
30(;3(5,0(176 The experiments were performed
using an electron beam with the energy of 42 MeV andthe macropulse duration of 47 ns. The reputation frequency of the macropulse of the electron beam was 30
Hz. Figure 1 shows a photograph of the ring resonator
used in the experiments. A hollow aluminum cylindricaltube with an inner diameter of 17.5 mm was installed as acollimator upstream the ring resonator. The electron beamOutput power [mV]

25
20
15
10
5
0
200

220

240

260

280

300

Time [ns]Fig. 2 THz-light power measured by the D-band
diode detector.

Fig. 1

Photograph of the ring resonator.

5()(5(1&(6>@ P. U. Jepsen HWDO., Laser Photonics Rev.  (2011) 124.
>@ M. Gensch HWDO., 3URF)(/1HZ<RUN , p.
474.
[3] N. Sei and T. Takahashi, Sci.Rep.  (2017) 17440.

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&2

+LJKFRXQWUDWH+HSRVLWLRQVHQVLWLYHGHWHFWRUUHDGRXWV\VWHP

S. Sato, K. Mori1, Y. Yoshino1, T. Seya, T. Otomo, H.
Oshita, K. Okawa2, N. Hikida2, K. Ishizawa2, A. Yamaguchi3, M. Matsuura3

700 ns, and it is a low-count-rate PSD (stopping gas: CF4,
3
He gas pressure: 20 atm.). The conditions are the same
except that the gas pressure is different. As shown inthese examples, the pulse width measurement function
can identify a high-count-rate PSD.

+LJK(QHUJ\$FFHOHUDWRU/DERUDWRU\.(.,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\
&DQRQ(OHFWURQ7XEHV 'HYLFHV&R/WG

&OHDU3XOVH&R/WG
,1752'8&7,21  Recently, the industrial use ofneutrons has become widespread, and compact accelerator-driven neutron sources have been used to develop
new materials. However, the development of neutron
detectors that support these experimental facilities has
been delayed. 3He gas detectors are the most reliable
neutron detectors and are typically utilized as position-sensitive detectors (PSDs) [1, 2]. However, thesedetectors have low count rates and low position resolutions. Therefore, joint research has begun between Canon
Electron Tubes & Devices Co., Ltd. (CETD), which
manufactures PSDs, and the High Energy Accelerator
Research Organization (KEK), which develops readout
circuits for neutron detectors.

,QWKLVUHVHDUFKZHDUHGHYHORSLQJWRLQFUHDVH
WKHFRXQWLQJUDWHRID+HJDVSRVLWLRQVHQVLWLYH
GHWHFWRU 36'  DQG D PD[LPXP FRXQWLQJ UDWH
RI  N FSV KDV EHHQ REWDLQHG :H UHSRUW WKHNH\ WHFKQRORJ\ RI D SXOVH ZLGWK PHWKRG WKDWKDVEHHQYHULILHGRIHIIHFWLYLW\DW.85
(;3(5,0(176 A pulse width measurement function is provided to diagnose whether a PSD can increase
the count rate. This technology [3] has been developed
for other detector systems. Figure 1 shows the pulse
width measurement method. The pulse width is obtainedby acquiring the pulse height from the pulse waveform.
To determine the pulse width, the counting starts from therising edge of the pulse and stops when it reaches half theheight of the pulse. The function has been verified at theB3 beam port in KUR.

Fig. 1.

(a)Fig. 2.

(b)
PHW graphs of (a) fast PSD and (b) slow PSD

Various techniques are necessary to increase the counting
rate of the 3He neutron detector, and the pulse width
method is an essential technique. KUR is the optimal
neutron generator to verify this method.

5()(5(1&(6[1] 66DWR HW DO (3- :HE &RQI 8&$16KWWSVGRLRUJHSMFRQI.
[2] S. Satoh HW DO, NIMA, , 103–106 (2009), DOI
10.1016/ j.nima.2008.11.054.
[3] S. Satoh, Physica B, 551, 401–404 (2018), DOI
10.1016/j.physb.2018.03.011.

Pulse-width measurement method5(68/76 Figure 2 shows the pulse height versus
width (PHW) graphs using the pulse width measurement
function. The vertical axis is the pulse width (25 ns perchannel), and the horizontal axis is the pulse height. Figure 2(a) shows that the entire signal gathers around 280
ns along the vertical axis, and it is a high-count-rate PSD(stopping gas: CF4, 3He gas pressure: 6 atm.). Figure 2(b)shows that the low pulse height signal extends to around

31044

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&2

1HXWURQDFWLYDWLRQDQDO\VLVRI$ULQWLWDQLXPPHWDO

T. Miura, N. Yoshinaga1, Y. Iinuma1 and S. Sekimoto1
1DWLRQDO0HWURORJ\,QVWLWXWHRI-DSDQ$,67,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFHV.\RWR8QLYHUVLW\,1752'8&7,21  National Metrology Institute ofJapan (NMIJ) is responsible for developing certified reference materials and for establishing the traceability of SI(The International System of Units) on chemical metrology in Japan. To establish SI traceability, the primarymethod of measurements should be applied to the characterization of the certified reference materials. Recently,
neutron activation analysis using comparator standard isrecognized as a potential primary ratio method [1]. Despite the potential of neutron activation analysis as primary ratio method, the evaluation of the measurement
uncertainty is required in any analysis. In general, there
are three main components of uncertainty in neutron activation analysis, that is, sample preparation uncertainty,
neutron flux homogeneity, and gamma ray measurement
uncertainty. Usually, flux monitor is used to correct theneutron flux in-homogeneity. However, although the flux
monitor can correct the neutron flux variation using thecount rate of the known amount of the monitor nuclide, itdoes not reflect the neutron flux of the actual sample.
The most practical method to eliminate neutron flux
in-homogeneity and to improve gamma ray measurement
uncertainty is an internal standard method [2, 3]. For thedevelopment of primary inorganic standard solution as
national standard, the purity of starting material has to be
determined. The high purity Ti metal was candidate
starting material for preparation of titanium standard solution as national standard of Japan. The several trace
analytical methods including neutron activation analysis,
were used for purity determination of the high purity Ti
metal. In this work, we presented that capability of instrumental neutron activation analysis for determinationof Ar in high purity Ti metal.
(;3(5,0(176 The high purity Ti metal was purchased from Sumitomo Metal Mining Co. Ltd. The informative purity value of the Ti metal was 99.9 %. The
ambient air in pre-cleaned 1 mL volume of PFA (Perfluoroalkoxy alkanes) vials were used as Ar calibration
standard. The volume of PFA vials were calibrated byweighing mass of pure water prepared from Mill-Q Advance pure water system filled in each vial. The calibration of volume Mettler Toredo XP205 semi-micro balance was used for volume calibration. The calibrated
PFA vials were heat sealed into Al coated polyethylene
bags. One hundred mg of the Ti metal samples were used
for Ar analysis. The neutron irradiations were performed
by KUR (Kyoto University Research Reactor) Pn3(thermal neutron flux: 4.7 x 1012 cm-2s-1) for 2 min.

The J ray measurement system consisted of an ORTEC
GEM 30-76-LB-C-HJ Ge detector and a multichannel
analyzer SEIKO EG & G MCA 7. Because theshort-lived radioactive nuclide 20F (t1/2=11 s) was produced in PFA vial by neutron irradiation, the gamma ray
measurement was started after 15 min.
5(68/76 The stable isotope 40Ar produce radioactive
nuclide 41Ar by neutron irradiation. Usually, air contain0.93 % of Ar. Hence, air in PFA vial can be used for calibration standard for Ar.
In this experiment, Ar in the high purity Ti metal
sample could not be detected by instrumental neutron
activation analysis. Therefore, the upper limit of Ar in thehigh purity Ti metal sample were estimated from thecount rate of energy region of gamma rays emitted by
41
Ar induced radioactive nuclide. The estimated upper
limit of Ar were <4.010-8 g/g.
Table Analytical results of Ar in high purity Ti metal
Sample
Ti-a
Ti-b
Ti-c
Ti-d
Ti-e
Ti-f

Ar g/g< 4.610-8< 3.010-8< 2.610-8< 3.510-8< 4.110-8< 4.010-8

5()(5(1&(6>@ R.Greenberg, P. Bode, E. De Nardi Fernandes, Spectrochim. Acta B, 66 (2011) 193-241.
>@ T. Miura, K.Chiba, T. Kuroiwa, T. Narukawa,
A.Hioki,+ Matsue, Talanta, 82 (2010) 1143-1148.
>@ T. Miura, R. Okumura, Y. Iinuma, S. Sekimoto, K.
Takamiya, M. Ohata, A.Hioki, J. Radioanal. Nucl.
Chem., 303(2105), 1417-1420.
>@ NuDat 2, National Nuclear Data Center inLaboratory,
Brookhaven
National
https://www.nndc.bnl.gov/nudat2/index.jsp

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&2

A response of inner-through type ionizaiotn chamber to 41Ar

A. Yunoki, H. Yashima1, R. Okumura1 and T. Yamada2
National Metrology Institute of Japan, National Instituteof Industrial Science and Technology
1Institute for Integrated Radiation and Nuclear Science,
Kyoto University
2
Kindai University Atomic Energy Research Institute
INTRODUCTION: Equipment for continuous monitoring of radioactivity in gaseous effluents are widelyused in nuclear power plants and other radiation facilities.
A response of the equipment to radioactive gas is one of
the most important characteristics. It is usually checkedby using a sealed solid source, however, a test using radioactive gases is necessary when testing a newly developed equipment and calibrating an equipment for
maintenance. In the test, the radioactive gas whose activity per unit volume is known is supplied to the equipment.
Then, the response is obtained by dividing the indicationof the equipment by the activity per unit volume. The
activity per unit volume can be determined by using a setof proportional counters, however, this measurement israther complexed and is not suitable for product tests. To
solve this problem, the inner-through type ionizationchamber, which is easier to handle, is used. The national
metrology institute of Japan (NMIJ) determined the response of the inner-through type ionization chamber(Ohkura ionization chamber: type I-4096 01/06) by using
a radioactive gas calibrated by the set of proportionalcounters. 85Kr has been used for testing the monitoring
equipment [1-3]. On the other hands, 133Xe and 41Ar areuseful for obtaining an energy dependence characteristic,
however, they are not commercially available. Especially,a half-life of 41Ar is only 109.6 minutes, therefore, measurement needs to be finished in several hours after production. Therefore, self-production of a radioactive argon(41Ar) by irradiating thermal neutrons to the stable argon(40Ar) is necessary. Accordingly, we produced 41Ar gas in
KUR-SLY and determined the response of the inner-through type ionization chamber by using the 41Ar
whose activity per unit volume was determined by the setof proportional counters.
SOURCE PREPARATION: The source of 41Ar was
prepared by the activating stable argon (40Ar) by irradiating thermal neutron. A research grade pure argon gas waspoured to a small vessel of crystal glass whose volume
was 10 cm3. A pressure of the gas was 300 hPa. The vessel was sealed with petroleum jelly. Then, the vessel wasplaced at the bottom of the KUR-SLY operating at 1 MW
for approximately 60 seconds. The nominal flux of thethermal neutron was 7.84×1011 [n-1 s-1 cm-2]. The 41Ar of
300 [kBq] was produced through 40Ar (n, J) 41Ar reaction.
The 41Ar was then transported to Kindai University
Atomic Energy Research Institute where a measurement
system was temporally installed.
MEASUREMENTS:

An activity of unit volume wasassessed by using a set of proportional counters connected in series. Conventional pulse counting electronics
were connected to the counters. The 41Ar diluted by P-10
gas (nominally argon 90% and methane 10%) was flown
through both the counters and the ionization chamber.
The designs of the counters are the same except for theirlength. In order to eliminate distortion of counts nearboth ends of the counter, the net count rate was usedwhich was obtained by subtracting a count rate obtainedby a shorter counter from that obtained by a longer counter. The activity per unit volume [Bq cm-3] was obtainedby dividing the net count rate by net volume of the counter. Temperature and pressure of the gas were monitored
during measurement to adjust the results to the standard
condition. For impurity assessment, an energy spectrumof gamma photon from the vessel containing the 41Ar was
obtained by using a high-purity germanium detector.
RESULTS: Fig. 1 shows the pulse count rate as a function of a volume of proportional counter. An activity perunit volume is derived from an inclination of approximate straight line obtained by the least square method.
The determined activity per unit volume was 85.3 Bq
cm-3. The output of inner through ionization chamber
flown by the 41Ar gas was 24.0 pA. Then, the response of
0.281 pA (Bq cm-3)-1 was obtained. The result was adjusted to the standard condition (20Υ, 101.3 kPa). As theresult of gamma photon spectrometry, an amount of impurity of the sample gas of 41Ar was negligible.

Fig. 1. Count rates as a function of a volume
of proportional counters.
41

Ar emits gamma photon of 1293.64 keV whose emission probability is 99.157 per 100 disintegration [4]. The
measurement will be improved by considering the effectof the photon to the measurement.
REFERENCES:[1] A. Yunoki, et. al., Applied Radiation and Isotopes, Vol.
68 (2010) pp.1340-1343.
[2] M Unterweger, L Johansson, L Karam, M Rodrigues
and A Yunoki, Metrologia 52 (2015) S156-S164.
[3] A. Yunoki, et. al., Applied Radiation and Isotopes, Vol.
134 (2018) pp.325-328.
[4] DDEP, URL: http://www.nucleide.org/DDEP_WG/
DDEPdata.htm.

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F. Tokanai, T. Moriya, T. Sumiyoshi, H. Kondo, H.
Sugiyama, M. Hayashi, T. OkadaDQG M. Hino)DFXOW\RI6FLHQFH<DPDJDWD8QLYHUVLW\*UDGXDWH 6FKRRO RI 6FLHQFH 7RN\R 0HWURSROLWDQ 8QLYHUVLW\

(OHFWURQ7XEH'LYLVLRQ+DPDPDWVX3KRWRQLFV..
,QVWLWXWH IRU ,QWHJUDWHG 5DGLDWLRQ DQG 1XFOHDU 6FLHQFH.\RWR8QLYHUVLW\
,1752'8&7,21  Neutron imaging is useful for
light elements in the sample such as hydrogen, lithium,boron, carbon, and nitrogen. Owing to their unique ability
to probe inside samples, neutrons have been widely utilized for neutron radiography in various fields, including
fundamental science, archaeology, and industry.
High position resolution with a moderate effective area
is required in practical applications of neutron imaging.
We have been developing a high-spatial-resolution neutron gas scintillation imager (n-GSI) with a capillary
plate gas detector (CPGD) [1,2]. It consists of a converter
layer of 10B4C, a CPGD filled with a Ne (90%) + CF4(10%) gas mixture, a mirror, lens optics, an imaging intensifier unit, and a CMOS camera. A 10B4C converter isdirectly mounted on the inlet surface of the CP. Charged
particles (D-rays and 7Li nuclei) are generated by a nuclear reaction between incident neutrons and the 10B. The
charged particles ionize the gas molecules and then generate electrons in the gas. The scintillation light is emitted
from the capillary holes upon gas excitation, simultaneously with electron multiplication. The scintillation lightfrom each capillary is read out as the imaging signal
through the optical mirror and lens system using an image intensified (II) CMOS camera.
Since the 10B converter is directly mounted on the inlet
surface of the CP, the track length of the charged particles is restricted to within the capillary. Thus, the spatial
resolution of incident neutrons is expected to be close to
the capillary diameter.
(;3(5,0(176 Fig. 1 shows the experimental setup.
The light yield and imaging capability of the n-GSI were
investigated using the cold neutron beam line CN-3 installed to the Kyoto University Reactor (KUR) [3]. The

neutron wavelength giving the maximum intensity andthe total flux of the CN-3 guide tube were 2 Å and 3.8 ×
106 neutron cm-2 s-1, respectively. The n-GSI system wasplaced 300 mm from the downstream exit of the neutron
guide. The neutrons were irradiated into a sample.
5(68/76 7KHQHXWURQWUDQVPLVVLRQLPDJHRID
FKDUDFWHUREWDLQHGZLWKWKHQ*6,LVVKRZQLQ)LJ 7KH H[SRVXUH WLPH IRU LPDJH ZDV  V Fig. 2
shows the anode currents of the n-GSI as a function of
the voltage across the CP electrode. The dependence oflight yield on the voltage of 'V is shown in Fig.3. The
light yields are defined as the total counts in the ROI-1
and ROI-2, respectively. The light yield increases exponentially with the gap voltage across the CP. This result
indicates that the n-GSI operates as a gas scintillation
proportional counter.
5()(5(1&(6>@ H. Kondo et al., Plasma Fusion Res. 13 (2018)
2406018.
>@ H. Kondo et al., Nucl. Instrum. and Methods. A 958(2020) 162804.
>@ M. Hino et al., Nucl. Instrum. and Methods. A 797(2015) 265.

)LJ([SHULPHQWDOVHWXSRIWKHQ*6,7KHUHJLRQ
RI LQWHUHVW 52, \HOORZ  DQG 52, UHG  DUH GH
ILQHG WR LQYHVWLJDWH WKH OLJKW \LHOG RI WKH QHXWURQWUDQVPLVVLRQLPDJH)LJ  Q*6, DQRGH FXUUHQW DV D IXQFWLRQ RI WKHYROWDJHDFURVVWKH&3HOHFWURGH

)LJ  1HXWURQ WUDQVPLVVLRQ LPDJHV DQG OLJKW\LHOGV DV D IXQFWLRQ RI WKH YROWDJH DFURVV WKH &3
HOHFWURGH

31080

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&2 *DPPDUD\PHDVXUHPHQWLQWKHEDVHPHQWRIWKH.\RWR8QLYHUVLW\5HVHDUFK5HDFWRUIDFLOLW\K. Okada, A. Fushimi, Y. Murakami, S. Sekimoto1, T.
Ohtsuki1, R. Okumura1

Measurement
device&HQWHUIRU7HFKQRORJ\,QQRYDWLRQ±(QHUJ\5HVHDUFK
DQG'HYHORSPHQW*URXS+LWDFKL/WG ,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\Cables(40 m)

Under the core

LaBr3(Ce)(;3(5,0(176 The measurement was carried out inthe heat exchanger room in the basement of the KUR
facility. Two gamma ray spectrometers were used, a highpurity germanium semiconductor detector (HPGe) and an
LaBr3(Ce) scintillation detector. Fig.1 shows the detector
positions. Dose rate given in the figure was estimated in apreviously done calculation[3]. The LaBr3(Ce) detector
was covered with a Pb shield having a collimator openedin the reactor core direction to measure the prompt gamma rays emitted from the reactor core. In order to measure the decay gamma rays around the LaBr3(Ce) detector,
the HPGe was covered with a shield having a collimatoropened in the LaBr3(Ce) direction.
The energy spectrum of gamma rays obtained with
the LaBr3(Ce) detector during 1 MW operation is shownin Fig.2. Total absorption peak of the 6130 keV gamma
ray which was emitted by decay of N-16 in the primarycooling system pipe was seen. Both the single escapepeak and double escape peak of the 6130 keV gamma ray
were confirmed. In addition, total absorption peak of the
511 keV gamma ray which was emitted by decay of N-13
in the primary cooling system pipe were seen. The sum
peak of the 511 keV gamma ray was confirmed. Threepeaks were measured as other gamma rays. The energiesof the gamma ray peaks were about 4600 keV (a), about
4100 keV (b) and about 3600 keV (c).

HPGeHeat exchanger
room
Dose rateEV

1 MW 䠖䡚2 mSv/hFig. 1. Detector positions in the basement of the KUR
facility.
6130 keV

511 KeV

100

Count rate [cps],1752'8&7,21 Conventionally, fission chambers
are adopted as in-core detectors for neutron flux monitoring. Part of the current value of the fission chamber
during rated operation does not follow the instantaneouschanges of the reactor power because decay gamma raysfrom reactor structure materials and delayed gamma raysfrom fission products have a time lag for response.
However, it is difficult to separate neutron detection signals from gamma ray detection signals with a fission
chamber in a high dose rate environment. Therefore, weare considering a method that monitors the neutrons only
indirectly by measuring prompt gamma rays from thereactor core[1-2].
In the method, metal pieces are placed in a mixed
field of neutrons and gamma rays. The prompt gamma
rays emitted by the nuclear reaction between the neutrons
and the metals are measured. At this time, other gamma
rays around the reactor are interfering with measurements
made with gamma ray spectrometers located under thereactor vessel. In this study, we used the Kyoto University Research Reactor (KUR) facility to measure the gamma ray energy distribution under the reactor vessel toevaluate the interference gamma ray components.

Sum peak10

Double escapeSingle escape

Al

1
0.1

c

0.01

a
b

0.001

0

2000

4000
6000
Energy [keV]

8000

10000

Fig. 2. Energy spectrum obtained with the LaBr3(Ce)detector.
5(68/76  The energy calibration between 1022 keV(the sum peak of 511 keV) and 5108 keV (the double
escape peak of 6130 keV) was difficult because there wasno standard source to emit high energy gamma rays. In
addition, by taking into account that the energy resolutionof the LaBr3(Ce) detector was too low to analyze nuclides
in detail, we considered that these gamma rays werelikely to be prompt gamma rays emitted from Al whoseenergies were 4733 keV, 4111 keV and 3465 keV[4]. Al
was used as a material for a tank of the KUR. Therefore,
we attribute these observed gamma rays to the Al tank.
This Al tank is equivalent to a reactor pressure vessel (RPV) or a channel box in commercial reactors. The
RPV and channel box are made of stainless steel. Thus, incommercial reactors, prompt gamma rays originatingfrom stainless steel and decay gamma rays from N-13
and N-16 interfere with measurement. In the evaluationof applicability, it is necessary to estimate the influenceof the gamma rays originating from these reactor structures.
5()(5(1&(6[1] K. Okada HW DO., J. Nucl. Sci. Technol. ,
514-522(2020).
[2] K. Okada HW DO., KURNS progress report 2018
CO12-13 (2019).
[3] K. Okada HWDO., KURRI progress report 2012 CO3-3(2013).
[4] D L Anderson, HWDO., (ed), Kluwer Academic Publishers, Handbook of prompt gamma activation analysis with neutron beams, 190-364 (2004).

31089

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&2

1HXWURQHIILFLHQF\RIDWZRGLPHQVLRQDOQHXWURQGHWHFWRUZLWK033& 0SL[ H. Ohshita, H. Endo, T. Seya, Y. Yasu, M. Hino1, T. Oda1

neutron irradiation test is approximately 785.2±0.2 neutrons/s‧cm2. Furthermore, the counting rate of Mpix wasmeasured by replacing the helium-3 proportional chamber.
The neutron efficiency H is defined as follows,,QVWLWXWHRI0DWHULDOV6WUXFWXUH6FLHQFH.(.,QVWLWXWHRI,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\ε=,1752'8&7,21 The village of neutron resonancespin echo spectrometers (VIN ROSE) [1] is built in BL06
at the Materials and Life Science Experimental Facility(MLF). Mechanisms involving slow dynamics such as diffusion and relaxation in samples are observed by VIN
ROSE. VIN ROSE consists of two spectrometers; the Neutron Resonance Spin Echo (NRSE) spectrometer and Modulated Intensity by Zero Effort (MIEZE) spectrometer [2].
The MIEZE spectrometer measures a time beat signal depending on the operation conditions of two resonance spin
flippers. As it is well known, the MIEZE signal is modulated when a polarized neutron interacts with the magnetic
momentum of a sample. By spring 2020, we achieved the
MIEZE frequency of 800 kHz. In order to observe the slow
dynamics of a sample with high accuracy, a neutron detector with a suitable time resolution under 100 ns is required.
Therefore, we are developing a neutron pixel detector
called Mpix. Mpix is a medium-sized neutron detector andits active area is 320 mm×320 mm. The time resolution isunder 100 ns and the value is limited by the repetition of
the readout electronics. A 6LiF/ZnS (Ag) scintillator with
0.25 mm thickness is used as a neutron convertor. The detector also consists of 1024 Multi-Pixel Photon Counters(MPPCs) for photon counting [3]. Each MPPC is locatedby a 10 mm pitch, and consists of a 32×32 MPPC array. In
order to measure the neutron efficiency, the neutron irradiation test was performed in CN3 [4] at the Kyoto University Reactor (KUR). This paper describes the experimental
results of the neutron irradiation test.
(;3(5,0(176 DQG 5(68/76 Figure 1 shows theneutron irradiation tests to evaluate the detector performance of Mpix carried out from August 27 to August 29,
2019. The neutron efficiency of Mpix is introduced bycomparing with the measurement data of a helium-3 proportional chamber (3He gas filled pressure: 993 kPa). A
disk chopper is worked at 30 Hz to obtain the wavelength
dependence of the neutron efficiency of Mpix. Neutrons
from 1.5 Å to 4 Å, pass through the disk chopper. The helium-3 proportional chamber is set downstream at the distance of 1.221 m from the disk chopper. The detector isplaced in a neutron shielding case which is made from a
B4C resin. The size of the opening area of the neutron
shielding case is 1 cm2. The neutron intensity in CN3 isderived from the measurement data of the helium-3 proportional chamber with the absorption correction of the
SUS detector housing. Therefore, after the estimation of
the absorption correction with Geant4 [5], a toolkit to provide the simulation of the passage of particles through matter, the measurement data is converted to the neutron intensity. As a result, the expected neutron intensity in the

Where 1Mpix is the counting rate of Mpix and )n is the expected neutron intensity in CN3. The neutron efficiency of
Mpix is shown in figure 2. From the result, we found that
Mpix has a thermal neutron efficiency of approximately
21%. The neutron efficiency trends to increase linearly to
2 Å, and saturates beyond that value. This is caused by thecontribution of the absorption in the detector housing andthe neutron detection limitation with a 6LiF/ZnS (Ag) scintillator of 0.25 mm thickness. In future, we plan to further
evaluate the neutron efficiency by comparing the simulation results. This work has been carried out in part underthe visiting Researcher’s Program of the Institute for Integrated Radiation and Nuclear Science, Kyoto University.

Fig. 1 Overview of the experimental setup.

Fig. 2 Neutron efficiency of Mpix.
5()(5(1&(6[1] M. Hino HWDO, Physics Procedia,  (2013) 136-141.
[2] T. Oda HWDO, J. Phys. Soc. Conf. Proc., in press.
[3] Web page of Hamamatsu Photonics K. K., KWWSVKD
PDPDWVXFRPMSHQLQGH[KWPO.
[4] M. Hino HWDO, Annu. Rep. Res. Reactor Inst. Kyoto
Univ.  (1994) 196-204.
[5] S. Agostinelli HW DO, Nucl. Instr. and Meth. A (2003) 250-303.

31094

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5HVHDUFKRQ$FWLYDWLRQ$VVHVVPHQWRID5HDFWRU6WUXFWXUDO0DWHULDOVIRU'HFRPPLVVLRQLQJ  &2

M. Seki, K. Ishikawa, T. Sano1, H. Nagata, K. Ohtsuka,
T. Ohmori, H. Hanakawa, H. Ide, K. Tsuchiya,
Y. Fujihara2, J. Zhang2 and J. Hori2'HSDUWPHQWRI-075-DSDQ$WRPLF(QHUJ\$JHQF\$WRPLF(QHUJ\5HVHDUFK,QVWLWXWH.LQGDL8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21
The radioactive waste for decommission is usually solidified by alkaline cement fillers. However, hydrogen produced by reaction of aluminum (Al) with alkaline materials may damage the waste
body. Therefore, it is necessary to establish the treatment
technology of radioactive Al waste for safety management of the storage facility. Last year, the irradiated
Al alloy was successfully separated into relative
long half-life radionuclides and Al component by ourgroup.
In this study, the solution pH dependence of the nuclide coprecipitated with aluminum hydroxide (Al(OH)3)
was investigated for the purpose of recovering the Alcomponent as Al(OH)3.
(;3(5,0(176    At first, the impurities included
in an Al alloy separated it by filtration within cold examination. These solutions were analyzed of elementals
by ICP-AES.
Secondly, the Al samples were irradiated in Pn-2 of
KUR pneumatic transportation facility and cooled for 4
days. The irradiation condition and chemical composition of the sample are listed in Table 1 and Table 2, respectively. After the irradiation, sodium aluminate(Na[Al(OH)4]) was produced by dissolving the samples
in NaOH solution with pH of 5 - 11. The insoluble impurities included in the sample were separated by filtration. This solution was neutralized by hydrochloric acid(HCl) to precipitate as Al(OH)3. The radioactivity of the
impurities and Al(OH)3 were measured by a germanium
semiconductor detector so as to investigate chemical
behavior of the radionuclides.
Table 1 Irradiation conditions of sample in Pn-2.
Items
ValuesThermal power
5 MW
Thermal neutron flux
2.8 × 1017 m-2s-1
Epithermal neutron flux
1.1 × 1016 m-2s-1
Fast neutron flux
6.0 × 1016 m-2s-1
Irradiation time
20 min.
Cooling time
4 daysSample0.25 gTable 3 The results of Al recovery by ICP-AESղQuantity of afiltrate [mg]

ձ-ղ
[mg]

ճ
Recovery
[%]

5
100.0
0.40
7
100.0
<0.05*
9100.0<0.05*
11
100.0
13.70
* The detection lower limit value

99.60
99.95
99.95
86.30

99.6
100.0
100.0
86.3

pH

ձ
Meltability[mg]

Table 4 The results of radioactivity measurement withthe germanium semiconductor detector [Bq / Al-1g]
pH

5

Cr-51

1.67x10Na-24

2.11x107151.82x102.79x109142.36x101.85x1011
142.20x103.06x10

Si

Fe

Cu

Mn

Mg

Cr

Zn

Ti

0.61

0.42

0.28

0.02

0.99

0.24

0.01

0.04

1
4

&21&/86,21  The radionuclide which coprecipitated with Al(OH)3 were Cr-51 and Na-24Cl was included in the NaCl which was produced at the same time
when Al(OH)3was produced.
In future, an experiment scale would be scale up themodel and A more realistic processing condition is demanded.
5()(5(1&(6>@ Taichi Sato, Journal of the Mineralogical SocietyofJapan, 19(1), 1989, pp.21-41.
>@ Gitzen, W.H. (ed.), Alumina as a ceramic material.,
American Ceramic Society, 1970.
>@ M. Seki, et al., KURNS Progress Report, p.257,
2018

Table 2 Chemical Compositions of sample
rate
[%]

5(68/76
Table 3 shows the results of Al recovery
by ICP-AES. In pH = 7 and 9, the Al concentration ofthis solution was less than detection lower limit level.
In pH = 5 and 11, it was revealed that Al could becollected 85% or more as Al(OH)3. In addition, the NaCl
was produced with Al(OH)3 and included by Al(OH)3.
Secondly, a hot examination was conducted similarly. Al(OH)3 was measured radioactivity by a germanium
semiconductor detector after it was filtered and enoughto be wash with ion exchanged water. As a result, Cr-51
and Na-24 coprecipitated with Al(OH)3 were obtained.
Cr-51 was produced by a reaction of (n,γ) which was
impurities element of A6061. Na-24 was produced by
Al-27 (n, α) Na-24.
Cr-51was equal values under conditions of all. In
Na-24, pH = 5 is maximum, because there was muchproduced NaCl and quantity of Na-24 Cl was included in
Al(OH)3 more than other conditions.

31096 *ϓρνʖͶͺࣙ͟ਐ͹ࡀ୔൬ߺΝ‫͏͚ͫ͠ͱ͢ࡎى‬ɽ

‑279‑

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%HDP7HVWRIDPLFURFHOO0:3&IRUDPXRQHOHFWURQFRQYHUVLRQVHDUFKH[SHULPHQW'HH0H

+,=9<:>398,C7/>2C6+62+=,//8A/66589A8+8./B:/->/.
>99?>:/<09<7"+  $2/1+==C=>/7A+=79.303/.=9
>2+>63;?3.7/>2C6+6=2+66,/73B/.>9>2/<+8.3
73B/. 1+= A3>2 + :</-3=/6C -98><966/. 73B>?</ 0<+->398 
31?</ =29A=+-9<</6+>398,/>A//8./6+C/.0+6=/:?6=/
<+>/+8.+:?6=/2/312>90</+623>>2+>:<9.?-/.,C+8/6/-
6FKRRORI6FLHQFH2VDND8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH
><9823>>381>2<9?12>2/'!  $2/?83>90>2/./6+C/.
0+6=/:?6=/<+>/3=+<,3><+<C  $2/</.0366/.-3<-6/6+,/6/.
.\RWR8QLYHUVLW\)DFXOW\RI6FLHQFH2VDND&LW\8QLYHUVLW\+=  &-9<</=:98.=>9>2/=+7/-98031?<+>39890>2/1+=
,QVWLWXWHRI0DWHULDOV6WUXFWXUH6FLHQFH.(.A/9,>+38/.  90/003-3/8-C38>2/ 7/+=?</7/8>
$2/ ,6?/><3+816/ 6+,/6/. +=  & :<9@3./= >A9>37/=
2312/<1+=1+38A3>2>A9>37/==7+66/<./6+C/.0+6=/:?6=/
,1752'8&7,21  2+<1/.6/:>98 06+@9< @396+>398<+>/
& :<9-/== =?-2 +=   / -98@/<=398 &./-+C=+</2/+@36C=?::</==/.38>2/=>+8.+<.79./6
5(68/76  $2/:9=3>398+6</=96?>39890'!7/+=
90 :+<>3-6/ :2C=3-= #  9A/@/< 38 >2/ 79=> 90 >2/?</.A3>22312/</8/<1C>2+8>2+>A/?=/.38>2/:</@39?=
79./6= ,/C98. # 3> 3= -98=3./</. >9 ,/ 9--?<</. A3>2 +=>?.C=29A=,/>>/<@+6?/+8.3>3==?003-3/8>09<>2/:?<=></81>2 >2+> -+8 ,/ </+-2/. 38 >2/ -97381 /B:/<37/8>=
:9=/90///  ,/+7>/=>A3>2+:<9>9>C:/'!</
/// 3= 98/ 90 /B:/<37/8>= >2+> +37= >9 =/+<-2 09< /@/+6/.>2+>>2/./6+C/.0+6=/:?6=/-+8,/=?::</==/.,C 90 >2/
-98@/<=398 38 8?-6/+< 03/6. ) * +> + 6/@/6 90
?=3817/>2C6+673B/.<+8.3  1+=A236/7+38>+38
,<+8-2381 <+>39 38 >2/ =3816/ /@/8> =/8=3>3@3>C  > ?=/=
381 199. 1+= 1+38  $2/ 038+6 :/<09<7+8-/ =29?6. ,/2312:9A/< 2312:?<3>C :?6=/. :<9>98 ,/+7 0<97 !"
-2/-5/.,C?=381+:<9.?->398@/<=39890'!38"#  $2/ ./>/->9< 90 /// =29?6. ,/ 9:/<+>398+6 +0>/<
=0<97+,?<=>90:+<>3-6/=
D77:<9.?-/.,C>2/ :<9>98 :?6=/ 8 9<./< >9 =96@/ >2/ :<9,6/7 +7?6>3
A3</ :<9:9<>398+6 -2+7,/< '! A3>2 2312@96>+1/
=A3>-2381 >/-283;?/ A+= =?--/==0?66C ./@/69:/. ) * > 3=
@/<C 37:9<>+8> >9 37:<9@/ >2/ >9>+6 :/<09<7+8-/ 90 >2/
'! ,/09</ >2/ =>+<> 90 >2/ :2C=3-= .+>+ >+5381 +> !"389<./<09<,/>>/<:2C=3-==/8=3>3@3>CDelayed False Pulse Rate (Arbitrary) 953 ,/ ( 31+=2389  5/?-23 97?5+3  +1+9 +>9<3 ( #/3C+$ $+5+2+=23  $ $+5+2+=23   $/=237+  (+7+79>9
+8.#(+7+=238+(;3(5,0(176  $A9 /B:/<37/8>= A/</ :/<09<7/. 38
>23=03=-+6C/+< 8>2/ /B:/<37/8>>2<//'!=A/</=/;?/8>3+66C :6+-/. =9 >2+> >2/ ,/+7 /6/-><98= 0<97 >2/
%" #/6/-><98 23>>2<9?12+66>2<//90>2/7$2/
'! :/<09<7+8-/ A3>2 >2<// .300/</8> 1+= 73B>?</=+A/</ >/=>/. A2/</ 1+= 73B>?</= 90 <  3  "A/</        +8.     > 03<=> >2/ ,?<=>
8=  77 A3>2 /8/<1C ,//6/-><98=   /6/-><98=
381  /& A/</ 384/->/. >9 >2/ '!= +> >2/ >37381 31 9<</6+>398,/>A//8>2/./6+C/.0+6=/:?6=/<+>/+8.
A2/8 >2/C A/</ 38 >2/ 900=>+>/  $2/ '!= A/</ =318+61+38  #//>/B>09<79</./>+36= >?<8/.>998=>+>/<312>+0>/</+-2,?<=>+8.>2/+79?8>90
./6+C/. 0+6=/ :?6=/= 38.?-/. 98 >2/ </+.9?> /6/-><9./ 5()(5(1&(6=><3:= A/</ 7/+=?</. ,C ?=381 +=> =C=>/7 ) * ) *  $/=237+ 98 ,/2+60 90 >2/ /// 966+,9<+>398
/== ./6+C/. 0+6=/ :?6=/= A/</ =//8 += >2/ 73B>?</ 90 E////B:/<37/8>>9=/+<-209<7?98>9/6/-><98-98"+38-</+=/= /B>>2/,?<=>/6/-><98=A/</>?<8/.900 @/<=398 +> !" F 38 :<9-//.381= 90 %$ 

+8. >2/ '! /003-3/8-3/= A/</ 7/+=?</. A3>2 69A <+>/ -980/</8-/!9# ?+-> /6/-><98= +>  /& /8/<1C 0<97 >2/    $2/ ) *  +>9<3HWDOE0+=>2312@96>+1/=A3>-23817?6>3
>37/ +@/<+1/. /003-3/8-3/= +</    s   s A3</ :<9:9<>398+6 -2+7,/<F !<91 $2/9< B: !2C=
 
 

  +8.   s  09<   +8.  90 "
+
0<+->398= </=:/->3@/6C  38+66C >2/ /6/-><98 /8/<1C A+= ) * $<?981HWDOE"/+6$37/9==6/==97:</==398
38-</+=/.>9 /&+8.>2/:9=3>398</=96?>39890'! 90'+@/09<7=%=381+8!F$<+8= ?-6#-3
A+=7/+=?</. $2/;?3-5900638/+8+6C=3==29A=>2+>>2/  :9=3>398</=96?>3983=,/>>/<>2+8 77<7=38-6?.381>2/
7?6>3:6/ =-+>>/<381 /00/-> A23-2 3= =?003-3/8> 09< >2/ :2C=
3-=.+>+>+538138 /-98@/<=398=/+<-2 8 >2/  7/+=?</7/8> + :<9>9>C:/ '! A+= ?=/.
A3>2 7/>2C6+673B/. 1+= 38=>/+. 90 "
+ 73B/. 1+==38-/ >2/ 199.8/== 90 >2/ :/<09<7+8-/ 90 >2/ 398

‑280‑

&2

An attempt to produce carrier free tracer through photonuclear reaction
and hot atom effect

T. Kubota, K. Takamiya, S. Fukutani and Y. Shibahara
Institute for Integrated Radiation and Nuclear Science,
Kyoto University

INTRODUCTION: Photonuclear reactions can produce radioisotopes which are hardly produced throughneutron irradiation. The production reaction and its ratedepend on the energy of photons. Photons are usually
generated through the irradiation of high-energy electrons
to heavy metal. The KURNS-LINAC can accelerate electrons up to 46 Mev, hence in this limitation (γ, n) reaction
is dominant. The effective cross-section of this reaction isroughly 100 times as large as other reactions, such as (γ,2n), (γ, p), and (γ, np) reactions [1-2]. It is desirable thatthe (γ, n) reaction is used to produce radioisotopes. In thecase that radio isotopes are used for biological experiments as tracer, carrier free ones, whose specific activity
and purity is high, are required in order to avoid chemical
toxicity. However, carrier free isotopes cannot be produced through (γ, n) reactions because products are basically the same element as target. In order to solve thisdifficulty, the production of carrier free isotopes was attempted by hot atom effect. As an example, Shibata et al.
reported that a mixture of UO2 and NaCl was irradiatedwith neutrons and recoil fission products were trapped
inside soluble NaCl and were separated from insoluble
UO2 by adding water [3]. In this research radioisotopes
were produced through photon irradiation to a mixture ofoxides and salts.
EXPERIMENTS: Fe3O4 and MoO3 were used as oxide and NaCl and KCl as salt, and the composition of a
mixture is listed in Table 1. Each mixture was homogenized by grinding in a mortar and pestle and then was
encapsulated in a quartz test tube under vacuum. The
quartz test tube was irradiated with photons generated by
the bombardment of 30 MeV electrons to platinum sheetof 2 mm thick at the KURNS-LINAC. The platinum
sheet and quartz test tube were cooled by cooling waterand blowing air, respectively. The irradiation time islisted in Table 1. After the decay of short half-life nuclides in irradiated materials, they were transported to theTracer laboratory and subject to further treatment. The
mixture was added with water to suspension solution, andthis solution was transferred from the quartz tube to apolyethylene centrifugation tube. The quartz test tube waswashed twice with water, and the washing solution was
combined with the suspension solution. The centrifugation tubes were added with water to dissolve salt completely, shaken, and centrifuged to precipitate oxides. The
aqueous phase was separated from the residue phase. The
radioactivity of both phases was determined by
γ-spectrometry and yielded the fraction of radionuclide
produced from oxide phase to salt phase through a hot
atom effect.

Table 1 Irradiation condition
Sample ID
#1

#2*

Fe3O4

2.40 g0.90 gMoO3#3

0.14 g2.05 gNaCl

27.31 gKCl

0.91 gIrradiation time
12 hr
6 hr
1 hr
* An aliquot of the mixture was used for irradiation.
RESULTS: Irradiation of chloride provided Cl-34,
which was dominant radioactivity immediately after irradiation and was, however, trivial matter due to its shorthalf-life. On the other hand, irradiation of sodium provided long half-life Na-22, which was required to be removed, if necessary. The use of KCl was therefore desirable as binding salt. Table 2 shows the transfer fraction of
Fe-52 and Mo-99 from the oxide phase to the salt phase,as carrier free tracer of iron and molybdenum, respectively. The value of Fe-52 was calculated from the radioactivity of Mn-52, and was lower than the detection limit,
showing that no activated iron element was liberated
from iron oxide crystal. The value of Mo-99 was 3%;
however, during the water treatment the solution turned
to blue purple, showing the dissolution of matrix MoO3
and no longer carrier free solution. In conclusion the
production of carrier free tracer through photonuclear
reaction and hot atom effect requires alternative methods.
Table 2 Transfer fraction by hot atom effectSample ID

#1

#2

#3

Mixture

Fe3O4
NaCl

Fe3O4
KCl

MoO3
KCl

Tracer

Fe-52/Mn-52

Fe-52/Mn-52

Mo-99

Transfer
fraction

~0 %

~0 %

3%

REFERENCES:[1] T. Kubota et al., KURRI Progress Report 2014(2015).
[2] T. Kubota et al., KURRI Progress Report 2017(2018) 209.
[3] S. Shibata et al., Applied Radiation and Isotopes 60(2004) 625–628.

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R. Hazama, T. Yoshimoto, A. Rittirong, Y. Sakuma1, T.
Fujii2, T. Fukutani3, Y. Shibahara3

A new test tube method was studied with the same twophases stirred by hand (only a second), separated by acentrifuge with 3 min, and iterated for fifteen times. The
Ca concentration of both phases was measured by AAS
and its Ca transfer between the two phases and no loss tothe other medium was confirmed in Fig.2.

*UDGXDWH6FKRRORI+XPDQ(QYLURQPHQW2VDND6DQJ\R
8QLYHUVLW\
/DERUDWRU\IRU$GYDQFHG1XFOHDU(QHUJ\7RN\R,QVWLWXWHRI7HFKQRORJ\ 
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calcium has been studied in liquid-liquid extraction(LLE) with an appropriate crown-ether (CE) by utilizing
a conventional batch (macroscopic) method [1] and a
cutting edge micro-reactor/chip method [2]. Based on themeasured reaction time between organic and aqueous
solution seems fast (less than a minute) (Fig.1), a new
test tube method has been pursued and its Ca mass balance between two phases was confirmed (Fig. 2) as withthe case of batch and micro-reactor/chip methods.
(;3(5,0(176 Isotopic enrichment occurs according
to the following chemical exchange reaction:40
Ca2+(aq) +48CaL2+(org)Æ48Ca2+(aq) +40CaL2+(org)  (1)where L represents macrocyclic polyether(18-crown-6).
An aqueous solution (3M CaCl2) and organic solution(0.07M DC18C6 in chloroform) were stirred by a magnetic stirrer with changing a mixing time from 0 sec(no-mixing) to 60 min at room temperature and separated
with a constant standing time of 30 min. The Ca concentration for both phases was measured by AAS in Fig. 1.

Fig 1. The partition coefficient (Kpc) (= (Ca concentration in organic phase) / (Ca concentration in aqueous
phase) was measured by changing the mixing time of 0
(no-mixing), 30 sec and 1, 5, 10, 30, 60 min: Preliminary.

Fig 2. Ca concentration in aqueous phase (circle) andorganic phase (triangle) for the process of LLE. Iteration
is 15 times, zero is feed solution for CaCl2 aqueous andcrown-ether organic (CHCl3) phase: Preliminary.
5(68/76 It is noted that one process of this mixing/separation is only a few minutes and it takes less thanan hour for the total of fifteen times multistage process.
More than 3000 multistage enrichment process for ten
times enrichment of Ca natural abundance can beachieved for a week and the scale-up for the mass production with an order of ton size is also promising due tothis simple and easy handling procedure by utilizing thelab shaker and centrifugal separator in Fig. 3

Fig 3. An example of lab shaker (Right) and centrifugal
separator (Left).
5()(5(1&(6>@R. Hazama HWDO., KURRI Progress Report 2017, 104.
>@R. Hazama HWDO., KURRI Progress Report 2018, 252

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(;3(5,0(17$/ Vegetables, fish, mushroom, seaweeds, and wild plants were collected from
Ishinomaki farmers and fish markets mainly in
2017-2019. Samples were washed with tap water,
separated edible parts, freeze dried, and pulverized for
dried powder samples. NAA was done by three different
conditions according to nuclides for the interest. 1) One
portion of samples was irradiated for 1-1.5 min in TcPnsite. After 3 minutes decay, gamma spectrum wasmeasured for 10 minutes by Ge detector with CSS.
Levels of Br, Ca, Cl, I, K, Mg, Mn, Na, and V wereanalyzed using 80Br, 49Ca, 38Cl, 128I, 42K, 27Mg, 56Mn,
24
Na, and 52V. 2) Another portion of samples wasirradiated for 20 minutes, and gamma spec-trum wasmeasured for 20 minutes after 2-3 days decay for
analyzing As using 76As.
3) Another portion ofsamples was irradiated for 1 hour, and gamma spectrum
was measured for 20 minutes after 1month decay for analyzing Ag, Co, Cr, Cs, Fe, Rb, Sc, Se, and Zn using
76
As.1 h in the Kyoto University Reactor, Japan. Gamma-ray spectra of the irradiated samples were recorded
after one-month decay for 20-30 min using a Ge detector
system. Levels of Ag, Co, Cr, Cs, Fe, Rb, Sc, Se, and Zn
were obtained using 110mAg, 60Co, 51Cr, 134Cs, 59Fe, 86Rb,
46
Sc, 75Se, and 65Zn, respectively. NAA method used
was validated using NIST SRM 1570a Spinach
Leaves, NIST SRM 1566b Oyster Tissue, NIST SRM
1575 Pine Needles, NIST SRM 1573a Tomato Leaves,and NIST SRM 1548a Typical Diet.
Bioaccessible trace element levels in food samples
were estimated for several fish samples by using
an AOAC method. Briefly, about 1 g of dried oyster
soft tissue powders was incubated with α-amylase,protease, and amyloglucosidase one after another.
Water soluble dietary fiber was filtered from theundigested residue after adding ethanol, and both
fractions were analyzed by INAA.

5(68/76 Ag was found only in dried sakuraebi andami. I and V were found only in seaweeds. Several
data obtained for fish samples are shown in Table 1.
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Tuna
red muscle
Tunamedium fatty muscle
Skipjack tunawithout dark muscle
Skipjack tuna_
dark muscle
Salmon

&V

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0.31

35.8

2.75

16.8

0.20

22.4

2.11

13.5

0.15

38.1

2.17

21.8

0.20

313.6

12.38

25.9

0.45

11.4

2.32

11.7

From the results in Table 1, differences of Fe and Se levels between skipjack tuna muscle dark muscle and without dark muscle were remarkable.
Bioaccessible levels of Se in fish sample were obtained, and the ratios of bioaccessible Se to total Se were;0.45, 0.39, 0.51, 0.56, and 0.46 for tuna red muscle, tunamedium fatty muscle, skipjack tuna without dark muscle,
skipjack dark muscle, and salmon, respectively. It may
be said that about half of total Se is bioaccessible level.
Wild plants analyzed were; shidoke, Ostrich Fern,
alpine leek, fiveleaf aralia, Aralia sprout, udo, butterbur,
bracken, mizu, urui, bonna, Japanese parsley, and bamboo shoots from 4 different collection areas. Several
levels of elements in wild plants were interesting whencompared to ones of vegetables. For example, Mn levels in 13 species, except shidoke, fiveleaf aralia, andJapanese parsley, were high, though Mn levels in 32 vegetables were under the detection limit. Mn levels were
244 - 3620 mg/kg, DW in brackens, 2910 mg/kg, DW in
bonnna, 1540 mg/kg, DW in udo. Also, several elemental levels showed difference between collection area,and showed in Fig.1. Fig. 1 shows difference between
three shidoke collected from Yamagata Prefecture, Kahoku (Ishinomaki, Miyagi), and Kamaishi (Iwate Prefecture).
(OHPHQWDOOHYHOV PJNJ':)DFXOW\RI6FLHQFHVDQG(QJLQHHULQJ,VKLQRPDNL6HQVKX8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 It is important to obtain multi element levels in food samples for nutritional purposes.
For the analysis of multi elements in foodsamples, atomic absorption spectrometry (AAS) and
induced cou-pled plasma spectrometry (ICP-AES) are
widely used after pre-treatment of acid extraction oracid digestion. Though complete acid digestion isneeded for obtaining total levels of elements in foodsamples, it is not easy by the presence of highconcentrations of lipids, polysaccha-rides, HWF. preventing
acid digestion. For eliminating this problem, neutron
activation analysis was used for multi elements analysis
of Japanese food samples. Bioaccessi-ble trace elementlevels in soft tissues of oysters were also estimated byusing an AOAC method.

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H. Masui, T. Murase, M. Cho, S. Wei, C. Joseph andK.
Takamiya
/DERUDWRU\RI6SDFHFUDIW(QYLURQPHQW,QWHUDFWLRQ(Q
JLQHHULQJ.\XVKX,QVWLWXWHRI7HFKQRORJ\
1DQ\DQJ7HFKQRORJLFDO8QLYHUVLW\,QVWLWXWHIRU,QWHJUDWHG5DGLDWLRQDQG1XFOHDU6FLHQFH.\RWR8QLYHUVLW\,1752'8&7,21 
Commercial-Off-The-Shelf(COTS) Integrated Circuits (ICs) are mostly sensitive toirradiations (e.g., protons, heavy-ions, etc.) in space,leading to various Single-Event Effects (SEEs). Among
different SEEs, Single-Event-Latchup (SEL) is probably
the most critical because it is detrimental and often damages ICs[1, 2]. This paper reports a circuit implementation that serves to provide protection for COTS ICs from
SEL. Kyushu Institute of Technology (Kyutech) andNanyang Technological University (NTU) are conducting
a joint research program in 1U CubeSats project of
BIRDS-4. In BIRDS-4 project, LDAP(Latch-up Detection and Protection) developed by NTU as a part of themission of BIRDS-4[3] were installed (Fig. 1). LDAP
monitors the latch-up current occurred in a device andshutdowns the power line of the device. The on-groundhardware verification on the basis of 252Cf was demonstrated that the circuit successfully cuts off the SEL current and subsequently resets the COTS IC. The reported
circuit has been adopted in a 1U CubeSat that will belaunched early 2020.

Fig. 1 LDAP (Latch-up Detection and Protection)

Fig. 2 Circuit diagram and phot of setup(;3(5,0(176 Figure 2 shows the circuit diagram.
In this test, an AD converter was adopted as a sample,
and SEL was induced in the AD converter. A packageof the AD convertor was removed(=de-caped) forradiation from 252Cf. The AD convertor was set in thevacuum chamber and its pressure was less than 30
Pa. 252Cf source was mounted on XYZ stage and theposition of 252Cf was controlled from outside and was
moved above the sample. We checked whether LDAP
can detect the SEL and can cut the power line
connected the AD con-verter. To check the function of
LDAP, the actual latch-up current was measured with ameasuring instrument and the response of LDAP with aserial communication was monitored with PC1.
5(68/76 Figure 3 shows the current profile acquiredwith the measuring instrument. The current peak in thecurrent profile shows the current increasing due to SEL.
After the SEL, the current quickly recovered to the nominal current. This means that LDAP was able to detect the
SEL in the AD convertor and to reset the power line of
the AD convertor. In the same way, it was confirmed that
the LDAP correctly worked with the serial communication. Since the LDAP function was confirmed, LDAP was
installed on the mission board of the BIRDS-4 flightmodel. BIRDS-4 satellite will be launched in FY2020
and on-orbit demonstration will be planed.

Fig. 3 Latch-up current detection and recovery5()(5(1&(6>@ M. Cho et al., “Test and Verification of Nanosatellite
HORYU-II and Orbital Anomaly Investigation”, Aerospace Technology Japan,12 17-24, 2013.
>@ Tomioka et al., “Screening of nanosatellite microprocessors using californium single-event latch-up test results”, Acta Astronautica, 126, 334-341, 2016.
>@ https://www.birds-project.com/

31142
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‑289‑

1. Slow Neutron Physics and Neutron Scattering
PapersPotential-Dependent Structure of the Ionic Layer at the Electrode Interface of an Ionic Liquid Probed Using Neutron
Reflectometry
N. Nishi, J. Uchiyashiki, Y. Ikeda, S. Katakura, T. Oda, M. Hino and N. L. Yamada
The Journal of Physical Chemistry C 123 (14) (2019) 9223- 9230.
Current status of the neutron resonance spin echo spectrometer on BL06 䇾VIN ROSE䇿 at MLF, J-PARC
H. Endo, T. Oda, M. Hino and T. Hosobata
Physica B: Condensed Matter 564 (2019) 91- 93.
Elliptic neutron-focusing supermirror for illuminating small samples in neutron reflectometry
T. Hosobata, N. L. Yamada, M. Hino, H. Yoshinaga, F. Nemoto, K. Hori, T. Kawai, Y. Yamagata, M. Takeda and
S. Takeda
Optics Express 19 (2019) 26807.
A study of TOF-MIEZE reflectometry for nanomagnetic dynamics
M. Hino, T. Oda, H. Endo, N. L. Yamada, H. Seto, H. Ohshita and Y. Kawabata
Journal of Physics: Conference Series 1316 (2019).
Experimental test of 3He neutron-spin filter in MIEZE spectrometer
H. Hayashida, M. Hino, H. Endo, T. Oku, T. Okudaira, K. Sakai and T. Oda.
Journal of Physics: Conference Series 1316 (2019) 012013.
Focusing and imaging of cold neutrons with a permanent magnetic lensJ. T. Cremer, H. Filter, J. Klepp, P. Geltenbort, C. Dewhurst, T. Oda and R. H. Pantell.
Review of Scientific Instruments 91(1) (2020) 013704.
Structural and electrochemical features of (Li2S)x (SiS2)100䇵x superionic glasses
K. Mori, K. Iwase, Y. Oba, K. Ikeda, T. Otomo and T. Fukunaga
Solid State Ionics 344 (2020) 115141.
Proceedings
ᑠゅ X ⥺ᩓ஘ἲ䛻䜘䜛 DN-polymers 䛾ᵓ㐀ゎᯒ /SAXS study of the DN-polymers under different temperature and humidity atmosphere
T. Tominaga, R. Inoue, N. Sato and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb5-6, 2020) 19. (in Japanese)X ⥺ᑠゅᩓ஘ἲ䛻䜘䜛₶⁥Ἔ୰䛾ῧຍ๣䛾ゎᯒ/Structural analysis of lubricant additive using small-angle X-ray scattering
Y. Oba, M. Hino, N. Adachi, Y. Todaka, R. Inoue and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 20. (in Japanese)᰾ඹ㬆ᑠゅᩓ஘䛻䜘䜛㟁Ꮚ≧ែ䛾ᚤ⣽ᵓ㐀ほ ᡭἲ䛾㛤Ⓨ/
Nuclear resonant small-angle scattering for investigation of microstructures in electronic states
S. Kitao, M. Kurokuzu, Y. Kobayashi, M. Seto, Y. Yoda and S. Kishimoto
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 32. (in Japanese)
MPPC 䜢౑⏝䛧䛯஧ḟඖ୰ᛶᏊ᳨ฟჾ Mpix 䛾ᛶ⬟ホ౯ /Performance evaluation of a two-dimensional neutron detector with MPPC (Mpix)
H. Ohshita, H. Endo, T. Seya, Y. Yasu, M. Hino and T. Oda
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 40. (in Japanese)‑290‑୰ᛶᏊ‽ᙎᛶᩓ஘ ᐃ䜢⏝䛔䛯⁐፹౫Ꮡᛶ୺㙐䜙䛫䜣཯㌿䜢♧䛩㧗ศᏊ䛾ศᏊ䝎䜲䝘䝭䜽䝇䛾ゎ᫂/Elucidation of the molecular dynamics of the macromolecules exhibiting the solvent-depeibiting helix inversion byusing quasielastic neutron scattering measurement
Y. Nagata, M. Suginome, M. Sugiyama, R. Inoe, N. Sato and K. Morishima
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 43. (in Japanese)X ⥺ᑠゅᩓ஘ἲ䛚䜘䜃ືⓗගᩓ஘ἲ䛻䜘䜛₶⁥Ἔ୰⢓ᗘᣦᩘྥୖ๣䛾ᵓ㐀ゎᯒ/Structural analyses of viscosity index improvers in lubricant oil by means of dynamic light scattering and small angle
X-ray scattering
R. Takahashi, T. Hirayama, N. Sato, M. Sugiyama, Y. Takashima, T. Nakano and Y. Oba
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 44. (in Japanese)୰ᛶᏊ䛸 X ⥺䜢฼⏝䛧䛯」ྜ䜲䝯䞊䝆䞁䜾ᡭἲ䛾㧗ᗘ໬/Development of hybrid imaging technique using neutrons and X-ray
D. Ito, R. Okumura, K. Ito and Y. Saito
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 52. (in Japanese)X ⥺䞉୰ᛶᏊ཯ᑕ⋡ἲ䛻䜘䜛₶⁥⏺㠃䛾ᖹᆒᵓ㐀ホ౯/Investigation of lubrication interface by X-ray and neutron reflectometry
M. Hino, N. Adachi,Y. Todaka, Y. Oba, T. Hirayama, T. Oda, K. Oda, H. Endo and T. Hirayama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 55. (in Japanese)ᐇ㦂ᡭἲ䛸ィ⟬ᶵᡭἲ䛾⼥ྜ䛻䜘䜛⁐ᾮᩓ஘ἲ䛾᭱๓⥺/Mariage of computational and experimental techniques for solution small-angle scattering
R. Inoue, M. Sugiyama, N. Sato, K. Morishima, A. Okuda and R. Urade
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 56. (in Japanese)⟽ᆺ⮬ᕫ㞟ྜయ䛾Ỉ୰䛻䛚䛡䜛ືⓗ≉ᛶ/
Dynamic property of a box-shaped self-assembly in water
N. Sato, Y. Y. Zhang, Q. Jiang, T. Kojima, K. Morishima, T. Koide, M. Tachikawa, M. Sugiyama and S. Hiraoka
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 57. (in Japanese)ᑠゅᩓ஘䛸㉸㐲ᚰศᯒ䛾༠ዌⓗゎᯒ䠄AUC-SAS)䛻䜘䜛ᙅ఍ྜᛶ䝍䞁䝟䜽㉁」ྜయ䛾ᵓ㐀ゎᯒ/Structural analysis of weakly bound protein complex with concerted use of small angle scattering and analyticalultracentrifugation (AUC-SAS)
Ken Morishima, Maho Yagi-Utsumi, Rintaro Inoue, Nobuhiro Sato, Aya Okuda, Reiko Urade, Koichi Kato, andMasaaki Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 58. (in Japanese)X ⥺ᑠゅᩓ஘䛻䜘䜛኱㇋䝍䞁䝟䜽㉁䛾ᵓ㐀ゎᯒ/Nanostructural analysis of soy bean proteins by small-angle X-ray scattering
N. Sato, R. Urade, A. Okuda, K. Morishima, R. Inoue and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 59. (in Japanese)
KUR-IBS 䜢⏝䛔䛯ከᒙ⭷୰ᛶᏊ䝭䝷䞊㛤Ⓨ䛾⌧≧/
Current status of multilayer neutron mirror development with KUR-IBS
M. Hino, T. Oda, F. Funama, H. Yoshinaga, Y. Kawabata, T. Hosobata, M. Takeda, S. Ikebe and Y. Yamagata,
H. Endo and N. L. Yamada
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 60. (in Japanese)ᙉ┦㛵 f 㟁Ꮚ⣔㔠ᒓ㛫໬ྜ≀䛾⤖ᬗ䞉☢Ẽᵓ㐀䛾◊✲/Magnetic and crystal structure analyses on strongly correlated f-electron systems
Chihiro Tabata
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 64-65. (in Japanese)‑291‑

Reviews
100nm ᮍ‶䛾✵㛫ศゎ⬟䜢Ⓨ᥹䛩䜛㉸ᚤ⢏ᏊཎᏊ᰾ங๣䜢⏝䛔䛯෭䞉㉸෭୰ᛶᏊ᳨ฟჾ
㛗⦖┤ᓫ᪥ᮏ୰ᛶᏊ⛉Ꮫ఍ㄅ Ἴ⣠ 29(3) (2019) 133-137. (in Japanese)

2. Nuclear Physics and Nuclear Data
PapersNeutron total cross section measurements of polyethylene using time-of-flight method at KURNS-LINAC
J. Lee, J. Nishiyama, J. Hori, R. Kimura, T. Sako, A. Yamada and T. Sano
Journal of Nuclear Science and Technology 57(1) (2019) 1-8.
Measurements of Spallation Products Induced by Heavy Ions
H. Yashima and T. Nakamura
RADIOISOTOPES 68(8) (2019) 567-573.
X-ray pumping of the 229Th nuclear clock isomer
T. Masuda, A. Yoshimi, A. Fujieda, H. Fujimoto, H. Haba, H. Hara, T. Hiraki, H. Kaino, Y. Kasamatsu, S. Kitao, K.
Konashi, Y. Miyamoto, K. Okai, S. Okubo, N. Sasao, M. Seto, T. Schumm, Y. Shigekawa, K. Suzuki, S. Stellmer,
K. Tamasaku, S. Uetake, M. Watanabe, T. Watanabe, Y. Yasuda, A. Yamaguchi, Y. Yoda, T. Yokokita, M.
Yoshimura and K. Yoshimura
Nature 7773 (2019) 238-242.
Conceptual study on parasitic low-energy RI beam production with in-flight separator BigRIPS and the first stopping
examination for high-energy RI beams in the parasitic gas cellT. Sonoda, I. Katayama, M. Wada, H. Iimura, V. Sonnenschein, S. Iimura, A. Takamine, M. Rosenbusch, T. M.
Kojima, D. S. Ahn, N. Fukuda, T. Kubo, S. Nishimura, Y. Shimizu, H. Suzuki, H. Takeda, M. Tanigaki, H. Tomita,
K. Yoshida and H. Ishiyama
Progress of Theoretical and Experimental Physics 11 (2019) 113D02.
IMPROVEMENT OF GAMMA-RAY SUBTRACTION PROCEDURE FOR A CURRENT-MODE NEUTRONDETECTOR WITH A PAIR OF 6Li- AND 7Li-GLASS SCINTILLATORS
T. Matsumoto, A. Masuda, H. Harano, J. Hori and T. Sano
Radiation Protection Dosimetry ncz266 (2019) 1-6.
Experimental study of multiplex energy recovery internal target ring
H. Okita, A. Taniguchi, Y. Kuriyama, T. Uesugi, Y. Ishi, Y. Mori, M. Muto, Y. Ono, N. Ikeda, Y. Yonemura,A. Sato,
M. Kinsho, Y. Miyake, M. Yoshimoto and K. Okabe
Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors andAssociated Equipment 953 (2019) 162988.
Proceedings
Measurement of Temperature-dependent Thermal Neutron Spectrum in CaH2 Moderator Material for Space Reactor
J. Lee, T. Sano, J. Hori, T. Sako, R. Kimura, A. Yamada and J. Nishiyama
International Conference on Nuclear Data for Science and Technology (ND2019) Beijing, China (May19-24, 2019).
Neutron Capture Cross Section Measurement of Minor Actinides in Fast Neutron Energy Region for Study on
Nuclear Transmutation System
T. Katabuchi, J. Hori, N. Iwamoto, O. Iwamoto, A. Kimura, S. Nakamura, Y. Shibahara, K. Terada, K. Tosaka, S.
Endo, G. Rovira, Y. Kodama and H. Nakano
Proceedings of the 2019 Symposium on Nuclear Data Fukuoka, Japan (Nov.28-29, 2019).
MCS Multi-group Cross Sections Generationfor Fast Reactor Analysis
T. D. C. Nguyen䠈H. Lee䠈X. Du䠈V. Dos䠈T. Q. Tran and D. Lee
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 2-5.

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A Systematic Way to Determine Neutron Generation Size in Monte Carlo Simulation Accelerated by the CMFD
T. D. C. Nguyen, H. Lee䠈X. Du䠈V. Dos䠈T. Q. Tran and D. Lee
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 6-9.
Validation of Activation Analysis Methodon RWRVI of Kori Unitl using MCCARD/ORIGEN2
Y. l. Kim, S. H. Jang, D. H. Lee and H. J. Shim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 10-13.
Uncertainty Quantification of Neutronics Characteristics in Thermal Systems using Random Sampling
andContinuous Energy Monte-Carlo Methods
H. Oike, R. Kondo, T. Endo amd A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 14-17.
Peak Power Characteristics of Postulated Criticality in Fuel Debris
Y. Yamane
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 31-33.
Developmentoflntegral Kinetic Model with Delayed Neutrons Effect for Criticality Accident Analysis of Fukushisma
Daiichi NPP Fuel Debris
H. Takezawa䠈D. Tuya and T. Obara
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 34-35.
Radiation Dose by Criticality Accidents of Fuel Debris in Water
K. Fukuda, J. Nishiyama and T. Obara
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 36-39.
Development of Criticality Safety Evaluation Method Based on the Actual Dynamic Behavior of the Fuel Debris in
Water
T. Muramoto䠈J. Nishiyama and T. Obara
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 40-43.
Treatment of R-matrix Limited Formula in FRENDY
K. Tada and S. Kunieda
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 229-232.
Validation of New Fission Yield by Analysis of Post-Irradiation Examination
A. lso, S. Takeda and T. Kitada
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 233-235.
Continuous Thermal Neutron Scattering Data Processing Capability in RMC Code
L. Zheng, K. Wang and W. Wang
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 236-239.
Thermal neutron Scattering Data Generation Function in the nuclear Data Processing Code NECP-Atlas
Y. Tang, T. Zu䠈S. Yi, J. Xu and L. Cao
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 240-243.
Quantification of Effectiveness of lntegral Data Using Active Sub-Space in nuclear Data Testing
D. Imazato and G. Chiba
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 244-247.
Estimated Criticality Lower-Limit Multiplication Factor Considering Neutronic Similarity and Uncertainties ofEffective Multiplication Factor Using the Bootstrap Method(1) Teory
T. Hayashi䠈F. Nishioka䠈T. Endo and A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 250-253.
Estimated Criticality Lower-Limit Multiplication Factor Considering Neutronic Similarity and Uncertainties ofEffective Multiplication Factor Using the Bootstrap Method (2) Application
F. Nishioka, T. Hayashi䠈T. Endo and A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 254-257.

‑293‑

Covariance-Oriented Sample Transformation Method for Uncertainty Analysis
Z. Sui, L. Cao and C. Wan
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 258-261.
Effectiveness of Subcritical Measurement at Solid Moderated KUCA Corefor Reducing nuclear Data-Induced
Uncertainties in Other Light Water Reactor Analysis
T. Endo and A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 262-265.
Benchmark Study of Nuclear Processed Systems with NCA Data
S. Wada, K. Yoshida and T. Sugita
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 266-269.
Sensitivity Analysis for Generalized Response with RMC code
G. Shi, C. Jia, Q. Cheng and K. Wang
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 270-273.
Uncertainty Analysis of neutron Parameters for NESTOR
H. Liao, Q. Li, Y. Yu and Y. Hu
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 274-277.
Comparison of Methods of Generating Covariance Matrix of Fission Yield
K. Honta and G. Chiba
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 278-281.
App1ication of Surrogate Modeling with Singular Value Decomposition for Design Basis Accident Aiming
Statistical Safety Analysis
M. Matsushita, T. Endo and A.Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 282-285.
Preliminary Performance Assessment of the GPU Acceleration Modulein a Pinwise Core Thermal Hydraulics Code
ESCOT
K. M. Kim, N. Choi, J. Lee and H. G. Joo
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 288-291.
BEAVRS Benchmark Analysisbya Whole Core Transport Code nTER
H. Park and J. Y. Cho
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 292-295.
Initial Assessment of Anderson Acceleration on Pinwise Coupled Neutronics/Thermal-Hydraulics CodenTER/ESCOTJ. Lee䠈J. Y. Cho and H. G. Joo
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 296-299.
Pin-By-Pin Multi-physics Analysis and Evaluation of the Critical Heat Flux(CHF) in a PWR Core
J. Kim, K. S. Chaudri and Y. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 300-303.
Functional Expansion Tallies in Monte Carlo High Fidelity LWR Analysis
Bamidele Ebiwonjumi, Hyunsuk Lee, Peng Zhang and D. Lee
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 304-307.
Hybrid Parallelism of Internal Coupling Method between Monte Carlo Code RMC and Sub-channel ThermalHydraulic Code CTF
K. Li䠈S. Liu, J. Guo and K. Wang
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 308-311.
NECP-X and CTF Solutions to VERA Benchmark
B. Wang, Z. Liu and L. Cao
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 312-315.

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CRITICAL EXPERIMENT OF THORIUM LOADED THERMAL CORES AT KUCA (1) A NEW CRITICAL
EXPERIMENT OF THORIUM LOADED CORE WITH HARDER NEUTRON SPECTRUM IN KUCA
T. Sano, J. Hori, J. Lee, Y. Takahashi, K. Takahashi and H. Unesaki
Physics of Reactor Conference 2020 (PHYSOR2020) Cambridge, UK (Mar. 2020).
CRITICAL EXPERIMENT OF THORIUM LOADED THERMAL CORES AT KUCA (2) CRITICALITYANALYSIS OF THORIUM LOADED CORES IN KUCA
H. Unesaki, J. Hori, Y. Takahashi, J. Lee and T.Sano
Physics of Reactor Conference 2020 (PHYSOR2020) Cambridge, UK (Mar. 2020).
Experimental Study on Neutron Correlation Analysis for a Subcritical System Driven by a Pulsed Spallation Neutron
Source in KUCA
K. Nakajima, K. Takahashi, A. Sakon, S. Hohara, T. Sano, M. Yamanaka, C.H. Pyeon and K. Hashimoto
Physics of Reactor Conference 2020 (PHYSOR2020) Cambridge, UK (Mar. 2020).
▷ᑑ࿨ RI 䜢⏝䛔䛯᰾ศග䛸᰾≀ᛶ◊✲/
Nuclear spectroscopy and condensed matter physics using short-lived nuclei
Y. Ohkubo, A. Taniguchi, M. Tanigaki, M. Shibata, Y. Kojima, W. Sato, and S. Komatsuda
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 10-14. (in Japanese)
Reviews⇞ᩱ䝕䝤䝸᰾≉ᛶホ౯䛻㛵䜟䜛᰾䝕䞊䝍䝙䞊䝈䠉୰ᛶᏊ↷ᑕ䜺䞁䝬⥺䝇䝨䜽䝖䝹 ᐃ䠉ྡෆὈᚿ᰾䝕䞊䝍䝙䝳䞊䝇 122 (2019) 54-66.

3. Reactor Physics and Reactor Engineering
PapersAN IMPROVED PRESSURE CALCULATION METHOD FOR SIMULATIONS OF GAS 䇵 LIQUID TWOPHASE FLOWS ON UNSTRUCTURED MESHESK. Ito, T. Kunugi, T. Ezure, M. Tanaka, D. Ito and Y. Saito
Multiphase Science and Technology 31(2) (2019) 109-131.
Benchmarks of Criticality in Solid-Moderated and Solid-Reflected Core in at Kyoto University Critical Assembly
M. Yamanaka and C. H. Pyeon
Nuclear Science and Engineering 193 (2019) 404-416.
Experimental Analysis of Unique Combination-Number for the Third- and Fourth-order Neutron-Correlation Factors
in the Zero Power Reactor Noise
T. Endo, A. Yamamoto, M. Yamanaka and C. H. Pyeon
Journal of Nuclear Science and Technology 56(4) (2019) 322-336.
Measurements of the <sup>243</sup>Am Neutron Capture and Total Cross Sections with ANNRI at J-PARC
A. Kimura, S. Nakamura, K. Terada, T. Nakao, K. Mizuyama, N. Iwamoto, O. Iwamoto, H. Harada,T. Katabuchi,
M. Igashira, T. Sano, Y. Takahashi, C. H. Pyeon, S. Fukutani, T. Fujii, T. Yagi, K. Takamiya and J. Hori
Journal of Nuclear Science and Technology 56 (2019) 479-492.
Proton Beam Characteristics with Wavelength Shifting Fiber Detector at Kyoto University Critical Assembly
M. Yamanaka, K. W. Jang, S. H. Shin, C. H. Pyeon and B. Lee
Japanese Journal of Applied Physics 58 (2019) 036002-1_036002-6.
A Monte Carlo technique for sensitivity analysis of alpha-eigenvalue with the differential operator sampling method
T. Yamamoto and T. Sakamoto
Annals of Nuclear Energy 127 (2019) 178-187.
Effect of Neutron Spectrum on Subcritical Multiplication Factor in Accelerator-Driven System
N. Aizawa, M. Yamanaka, T. Iwasaki and C. H. Pyeon
Progress in Nuclear Energy 116 (2019) 158-167.

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Experiments on gas entrainment phenomena due to free surface vortex induced by flow passing beside stagnation
regionT. Ezure, K. Ito, M. Tanaka, H. Ohshima and Y. Kameyama
Nuclear Engineering and Design 350(15) 90-97.
First Nuclear Transmutation of 237Np and 241Am by Accelerator-Driven System at Kyoto University Critical
Assembly
C. H. Pyeon, M. Yamanaka, A. Oizumi, M. Fukushima, G. Chiba, K. Watanabe, T. Endo, W. F. G. van Rooijen, K.
Hashimoto, A. Sakon, N. Aizawa, Y. Kuriyama, T. Uesugi and Y. Ishi
Journal of Nuclear Science and Technology 56(8) (2019) 684-689.
Integral Experiments on Critical Irradiation of 237Np and 241Am Foils at Kyoto University Critical Assembly
C. H. Pyeon, M. Yamanaka, T. Sano and K. Takamiya
Nuclear Science and Engineering 193(9) (2019) 1023-1032.
Calculation of the Cross and Auto Power Spectrum Densities for Low Neutron Counting from Pulse Mode Detectors
A. Talamo, Y. Gohar, T. Yamamoto, M. Yamanaka and C. H. Pyeon
Annals of Nuclear Energy 131 (2019) 138-147.
Removal of Scale from Feed-water in Thermal Power Plant by Magnetic Separation-Analysis of Oxygenated Treatment ScaleM. Hiramatsu, J. Yamamoto, Y. Akiyama, F. Mishima, S. Nishijima, H. Okada, N. Hirota, T. Yamaji, H. Matsuura,
S. Namba, T. Sekine, Y. Kobayashi and M. Seto
Journal of Physics: Conference Series 1293(1) (2019) 012079.
Visualization of phase distribution in lead䇵bismuth eutectic during one-dimensional solidification process
D. Ito, H. Sato, Y. Saito, J. D. Parker, T. Shinohara and T. Kai
Journal of Visualization 22(5) (2019) 889-895.
An Impact of Inherent Neutron Source on Subcriticality Measurement in A Highly Enriched Uranium Core of Kyoto
University Critical Assembly
A. Sakon, T. Sano, S. Hohara, C. H. Pyeon and K. Hashimoto
Journal of Nuclear Science and Technology 56 (2019) 935-944.
Decomposition of neutron noise in a reactor into higher-order mode components and investigation of the space andfrequency dependence
T. Yamamoto and H. Sakamoto
Progress in Nuclear Energy 117 (2019) 103098.
Two-step Monte Carlo sensitivity analysis of alpha- and gamma-eigenvalues with the differential operator sampling
methodT. Yamamoto and H. Sakamoto
Annals of Nuclear Energy 133 (2019) 100-109.
Application of Linear Combination Method to Pulsed-Neutron Source Measurement at Kyoto University Critical
Assembly
R. Katano, M. Yamanaka and C. H. Pyeon
Nuclear Science and Engineering 193 (2019) 1394-1402.
Experimental study on local interfacial parameters in upward air-water bubbly flow in a vertical 6 × 6 rod bundle
X. Han, X. Shen, T. Yamamoto, K. Nakajima, H. Sun and T. Hibiki
International Journal of Heat and Mass Transfer 444 (2019) 118696.
Feasibility Study on Application of an Artificial Neural Network for Automatic Design of a Reactor Core at the
Kyoto University Critical Assembly
S. H. Kim, S. G. Shin, S. S. Han, M. H. Kim and C. H. Pyeon
Progress in Nuclear Energy 119 (2020) 103183.
Calculation of the Prompt Neutron Decay Constant of the KUCA Facility Configurations Driven by a Californiumof Spallation External Neutron Sources
A. Talamo, Y. Gohar, M. Yamanaka and C. H. Pyeon
Journal of Nuclear Science and Technology 57 (2020) 145-156.

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Estimation of Kinetics Parameters by Monte Carlo Fixed-Source Calculations for Accelerator-Driven System
H. J. Shim, D. H. Kim, M. Yamanaka and C. H. Pyeon
Journal of Nuclear Science and Technology 57(2) (2020) 177-186.
Experimental Analyses of beff / L in Accelerator-Driven System at Kyoto University Critical Assembly
M. Yamanaka, C. H. Pyeon, T. Endo, K. Watanabe, G. Chiba and W. F. G. van Rooijen
Journal of Nuclear Science and Technology 57(2) (2020) 205-215.
Measurement of Prompt Neutron Decay Constant with Spallation Neutrons at Kyoto University Critical Assembly
using Linear Combination Method
R. Katano, M. Yamanaka and C. H. Pyeon
Journal of Nuclear Science and Technology 57 (2020) 169-176.
Nuclear Data-Induced Uncertainty Quantification of Prompt Neutron Decay Constant based on Perturbation Theory
for ADS Experiments at KUCA
T. Endo, K. Watanabe, G. Chiba, M. Yamanaka, W. F. G. van Rooijen and C. H. P yeon
Journal of Nuclear Science and Technology 57 (2020) 196-204.
Paralyzable and Non-Paralyzable Dead-Time Corrections for the Neutron Detectors of the KUCA Facility using
External Neutron Sources
A. Talamo, Y. Gohar, M. Yamanaka and C. H. Pyeon
Journal of Nuclear Science and Technology 57 (2020) 157-168.
Real-Time Subcriticality Monitoring System based on A Highly Sensitive Optical Fiber Detector in An AcceleratorDriven System at the Kyoto University Critical Assembly
K. Watanabe, T. Endo and M. Yamanaka and C. H. Pyeon
Journal of Nuclear Science and Technology 57 (2020) 136-144.
Special Issue on Accelerator-Driven System Benchmarks at Kyoto University Critical Assembly
C. H. Pyeon, A. Talamo and M. Fukushima
Journal of Nuclear Science and Technology 57 (2020) 133-135.
Subcriticality Estimation by Extended Kalman Filter Technique in Transient Experiment with External Neutron
Source at Kyoto University Critical Assembly
M. Yamanaka, K. Watanabe and C. H. Pyeon
European Physical Journal Plus 135 (2020) 256-256.
Data Assimilation Using Subcritical Measurement of Prompt Neutron Decay Constant
T. Endo and A. Yamamoto
Nuclear Science and Engineering Selected papers from the 2019 M&C Conference (2020) 1-16.
Measurement of A Very Large Negative Reactivity Inserted by Rapid Withdrawal of A Partial Fuel Loading in Kyoto
University Critical Assembly
A. Sakon, T. Sano, K. Takahashi, K. Nakajima, S. Hohara, C. H. Pyeon and K. Hashimoto
Journal of Nuclear Science and Technology 57 (2020) 335-343.
Proceedings
Parametric analysis of bubble and dissolved gas behavior in primary coolant system of sodium-cooled fast reactors
K. Matsushita, K. Ito, T. Ezure and M. Tanaka
27th International Conference on Nuclear Engineering: Nuclear Power Saves the World!, ICONE 2019
Ibaraki䠗 Japan (May19-24, 2019).
Study on numerical simulation of void fraction profile in LBE two-phase flow
K. Maeda, G. Ariyoshi, D. Ito, K. Ito and Y. Saito
27th International Conference on Nuclear Engineering: Nuclear Power Saves the World!, ICONE 2019
Ibaraki䠗 Japan (May19-24, 2019).
Study on evaluation method for entrained gas flow rate by free surface vortex
K. Ito, D. Ito, Y. Saito, T. Ezure, K. Matsushita, M. Tanaka and Y. Imai
18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics, NURETH 2019 Portland, Oregon, USA(Aug.18-23, 2019) 6632-6642.

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Two-phase flow structure in a particle bed packed in a confined channel
D. Ito, T. Kurisaki, K. Ito, Y. Saito, Y. Imaizumi, K.-I. Matsuba and K. Kamiyama
18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics, NURETH 2019 Portland, Oregon, USA(Aug.18-23, 2019) 6430-6439.
Measurement of Gamma Rays from Radiative Capture of Uranium-238 and Decay of Short Lived Fission Products
from Subcritical System
Y. Nauchi, T. Sano, H. Unesaki, S. Sato, M. Suzuki and H. Ohta
11th International Conference on Nuclear Criticality safety (ICNC2019䠅Paris, France (Sept.15-20, 2019).
Conversion from Prompt Neutron Decay Constant to Subcriticality Using Point Kinetics Parameters Based on Alphaand keff-eigenfunctions
Y. Nauchi, T. Sano, H. Unesaki, S. Sato, M. Suzuki and H. Ohta
11th International Conference on Nuclear Criticality safety (ICNC2019䠅Paris, France (Sept.15-20, 2019).
Measurements of subcriticality in dollar units using time-domain decomposition based integral method
A. Nonaka, T. Endo, A. Yamamoto, M. Yamanaka, T. Sano and C.H. Pyeon
11th International Conference on Nuclear Criticality safety (ICNC2019䠅Paris, France (Sept.15-20, 2019).
Ỉᖹ⟶⩌ෆ✵Ẽ-Ỉ஧┦ὶ䛾⇕ὶື≉ᛶ䛻ཬ䜌䛩䝢䝑䝏┤ᚄẚ䛾ᙳ㡪䛻㛵䛩䜛◊✲/Effect of Pitch-to-Diameter Ratio on Heat Transfer and Flow Characteristics of Air-Water TwoPhase Flow in
Horizontal Tube BundleⲨᮌ ᓙஓ, ᮧᕝ ⱥᶞ, ᮡᮏ ຾⨾, ὸ㔝 ➼, ఀ⸨ ኱௓/
K. Araki, H. Murakawa, K. Sugimoto, H. Asano and D. Ito➨ 24 ᅇ ືຊ䞉䜶䝛䝹䜼䞊ᢏ⾡䝅䞁䝫䝆䜴䝮[in Japanese] Tokyo, Japan (July20-21, 2019) E144.
Experimental Analyse䡏 of Spallation Neutrons By 100 MeV Protons and Lead䠉Bismuth Target at Kyoto University
Criticality Assembly
K. Morioka䠈M. Yamanaka䠈K. Sugiura and C.H. Pyeon
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 19-21.
Applicability of Extended Kalman Filter Teclmique to Reactivity Monitoring at Kyoto University Criticality
Assembly
M. Yamanaka and C. H. Pyeon
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 22-25.
Core Design of Accelerator Driven System with Reactivity Control Method using Thorium
K. Nakamura䠈H. Saito䠈N. Aizawa and T. Iwasaki
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 26-29.
BEAVRS Benchmark Simulation by using NECP䠉Bamboo
J. Yang䠈H. Wu and Y. Li
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 47-50.
Optimization and Verification of PWR Pin-by-pin Fuel Management Calculation Code NECP 䠉Bamboo2.0
S. Wang䠈L. Cao䠈Y. Li and W. Yang
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 51-54.
Application of cosKERNEL Code for NPP Shielding Calculation
W. Song, Y. Sun, S. Li, X. Wang, H. Yu and Y. Chen
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 55-57.
GPU/CPU Concurrent Heterogeneous Parallel MOC Calculation with Asynchronous Communication Scheme
L. Liang䠈P. Song䠈Q. Zhang䠈Z. Zhang and Q. Zhao
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 58-61.
Impact of Diffusion Coefficient and Correction Term on the Convergenceof CMFD Acceleration for MOC
Y. Oshima, T. Endo and A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 62-65.

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Application of Improved Tone
X. Du, S. Choi, J. Choe, W. Lee and D. Lee
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 66-69.
Application of the SuPer-Homogenization Method in Fast Reactor Analysis System SARAX
L. Wei, Y. Zheng, B. Xiao, L. Xu and H. Wu
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 70-73.
Progress on Multi-physics Calculations of Nuclear Reactor Cores with the IGA Method
W.F.G. van Rooijen
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 74-77.
Research on a Method for Self-Shielding Calculations Based on IGA-Method
M. Nezondet and W.F.G. van Rooijen
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 78-81.
Study on Effective Cross Section of Pu Spot in MOX fuelT. Kawano䠈S. Takeda䠈T. Kitada, Y. Ohoka, S. Matsuoka and H. Nagano
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 82-85.
Modification of MOC for Considering Double Heterogeneity due to Pu Spots in MOX Fuel
A. Ogawa䠈H. Yamaguchi䠈S. Takeda䠈T. Kitada䠈Y. Ohoka, S. Matsuoka and H. Nagano
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 86-89.
Homogenization Analysis of double-Heterogeneous Fuel and Bumable Poison
L. Lou, Y. Dong, C. Xiaoming, Y. Yingrui and P. Xingjie
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 90-93.
Prediction Analysis of 243Am/235U Solid Fission Rate Ration at KUCA solid Moderator Core
T. Sano, J. Hori and Y. Takahashi
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 94-97.
Effect of neutron Absorber on Production of Plutonium238 for BWR Assembly
H. Ohuchi, S. Takeda and T. Kitada
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 99-102.
Study on the Optimization of Assembly Design of Single-Pass Supercritical Water-Cooled Fast Reactor
L. Huang, Z. Liu and X. Wang
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 103-107.
Application of Direct Simulation Method for neutron Space-Time Kinetics Based on RMC
J. Lijun, S. Xiaotong, G. Xiaoyu and W. Kan
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 108-111.
Core Design of a Molten Salt Reactor with Chloride Fuel
M. Watanabe and W.F G. van Rooijen
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 112-115.
Monte Carlo Based Analysis for CANDLE Burning Reactor
H. H. Nguyen䠈J. Nishiyama and T. Obara
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 116-118.
Verification of FRBurner Module of CBZ Code System Based on OECD/NEA Benchmark Report
J. Fan and G. Chiba
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 127-130.
Development of a Steady-State Core Analysis Code System for VVER
L. Yu 䠈G. Chen, J. Bao䠈L. Wei䠈Z. Liao and S. Zhang
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 131-134.
BEAVRS Benchmark Evaluations with Studsvik CMS5 Code Package
T. Bahadir and M. Yamasaki
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 135-138.

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An Improved Chebyshev Rational Approximation Method Base on Order Reduction of Krylov Subspace Method
Y. Hu, Q. Luo, D. Yao, Y. Yu, H. Liao and B. Zhou
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 139-142.
Improvement of Optimally-Weighted Predictor-Corrector Method for Nuclear Fuel Burnup Calculations
J. Sasuga, G. Chiba, Y. Ohoka䠈K. Yamamoto and H. Nagano
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 143-146.
Robustness of the GPS Functions in Pinwise Neutronics Analysis of PWRs
H. Yu and Y. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 147-150.
APEC-corrected NEM Analysis of the VERA Core
S. Jang, K. Lee and Y. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 151-154.
Discontinuity Factor䠗A Discontinuity Condition for Angular Flux?
A. Yamamoto and T. Endo
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 155-157.
Calculation of Higher Eigen-modes of the Forward and Adjoint neutron Diffusion Equations Using IRAM Algorithm
Based on Domain Decomposition
W. Wu, Y. Yu䠈Q. Luo䠈D. Yao䠈Q. Li and X. Chai
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 158-161.
Performance of the RSE䠄Resonace calculation using energy Spectral Expansion䠅 Method for Heterogeneous Pincell Geometry
R. Kondo䠈T. Endo䠈A. Yamamoto, S. Takeda, H. Koike, K. Yamaji and D. Sato
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 162-165.
Application of Singular Value Decomposition and Low Rank Approximation for Compression of Macroscopic andMicroscopic Cross Section Table for Core Calculations
M. Yamamoto, T. Endo and A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 166-169.
Compression of Multi-Physics SimUlation OutPut Data Using Principle Component Analysis
A. Cherezov, J. Park, H. Kim, N. S. M. Ali and D. Lee
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 170-174.
Refinement of Convolutional Neural Network for Neutronic Design Parameter Prediction of a Loading Pattern
H. Jang, H. C. Shin and H. C. Lee
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 175-178.
Experimental Validation for the Pi n- wise Isotope Prediction Methodology
M. Lee, T. Noh and M. H. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 179-182.
The neutron Streaming Correction Method in the Homogenization of Pebble-bed HTGR Reflector
Y. Wen, D. She, L. Shi and J. Zhao
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 183-186.
App1ication of neutron Balance Analysis in Enhancing the Temperature Reactivity Feedback of Gas-cooled Fast
Reactor
C. Zhang, Y. Zheng and L. Wei
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 187-190.
Innovative Design Concepts of Bumable Poison Rods for PWR
A. Dandi and M. H. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 191-195.
Research on Core Design of Pebble Bed Advanced High Temperature Reactor
W. Lianjie, S. Wei, X. Bangyang, Z. Yang and Y. Rui
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 196-199.

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C5G7-TD Benchmark Analysis using Multigrid Amplitude Function Method
K. Tsujita, T. Endo and A. Yamamoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 201-204.
Fast (Floating Absorber for Safety at Transient䠅for the Improved Safety of MOX -loaded Sodium-cooled Fast
Reactors
C. Kim and Y. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 205-208.
A Comparative Study on the lQS (Improved Quasi-Static) and PCQS (Predictor Cor Mtor Qusai-Static) Methods
T. Oh, Y. Chung and Y. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 209-212.
Point Kinetics Analysis for Source-jerk Experimentat AGN‐201K
S. Lim, H. J. Shim and M. H. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 213-215.
A Subcriticality Measurement of AGN䠉201K Reactor Using the Rossi-q Method
S. Moon, J. H. Kim, M. H. Kim and S. G. Hong
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 217-220.
Experiment using a Random Selection Method for AGN-201K
J. H. Kim, S. H. Moon, S. G. Hong and M. H. Kim
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 221-224.
Education on Reactor Physics and Fuel Cycle using Experimental Facilities of the Nuclear Industry
K. Yoshioka䠈T. Sugita䠈S. Wada䠈R. Kimura䠈Y. Yamashita䠈H. Kumanomido, T. Masuyama, M. Akiyama, H.
Miyadera and K. Hiraiwa
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 225-227.
Neutron Correlation Analysis for a Subcritical Reactor System Driven by a Pulsed Spallation Neutron Source in
KUCA
K. Nakajima, A. Sakon, S. Hohara, K. Takahashi, M. Yamanaka, T. Sano, C.H. Pyeon and K. Hashimoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019).
A Correlation Characteristics of Spurious Counts of Fission Counter Installed in Kyoto University Reactor for
Reactor Operation
S.y. Hohara, A. Sakon, T. Sano, K. Nakajima, K. Takahashi and K. Hashimoto
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019).
䝫䞁䝥ෆẼἻᣲື䛾ᩘ್ゎᯒ䛸 X ⥺䜲䝯䞊䝆䞁䜾/
Numerical simulation and X-ray imaging of entrapped gas bubble behavior in coolant pump
R. Xiong, K. Ito, D. Ito and Y. Saito
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 33. (in Japanese)⌫඘ሸᒙෆ䛻䛚䛡䜛Ẽᾮ஧┦ὶ≉ᛶ䛻ᑐ䛩䜛㓄⟶ᚄ䛾ᙳ㡪 /Effect of pipe diameter on gas-liquid two-phase flow characteristics in a spherical packed bed
A. Ishikuro, D. Ito, K. Ito and Y. Saito
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 34. (in Japanese)
A two-phase flow database in a light-water-reactor-simulated rod bundle
X. Han, X. Shen, T. Yamamoto, K. Nakajima and T. Hibiki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 46. (in Japanese)⇕㟁ኚ᥮ 䠉ᇶ♏,ᛂ⏝,ᮦᩱ䠉/
Thermoelectrics -fundamental, applications and materialsK. Kurosaki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 66-67. (in Japanese)᰾◚○୰ᛶᏊ※䜢⏝䛔䛯ຍ㏿ჾ㥑ື䝅䝇䝔䝮䛻㛵䛩䜛ᇶ♏◊✲/Basic Basic research of accelerator-driven riven system with spallation neutrons
C. H. Pyeon, M. Yamanaka, K. Hashimoto, N. Aizawa, K. Watanabe, G. Chiba and and A. Oizumii
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 68-70. (in Japanese)‑301‑

Reactor Noise Analysis for a Graphite-moderated and -reflected core in KUCA
A. sakon, K. nakajima, K. takahashi, S. hohara, T. sano, Y. fukaya and K. hashimoto
PHYSOR 2020: Transition to a Scalable Nuclear Future Cambrige, United Kingdom (Mar., 2020).

4. Material Science and Radiation Effects
Papers
Effect of Y2O3 particles on the helium ion irradiation damage of W-2%Y2O3 composite prepared by wet chemical
methodY. Gang, L.L. Ma, T.X. Yue, Z. Xiang, Q. Xu, Z.X. Yong, L.E. Yang, C.X. Zhong, C.J. Gui and W.Y. Cheng
Materialia 6 (2019) 100268.
Microstructure and Its High Temperature Oxidation Behavior of W-Cr Alloys Prepared by Spark Plasma Sintering
Q.Q. Hou, K. Huang, L.M. Luo, X.Y. Tan, X. Zan, Q. Xu, X.Y. Zhu and Y.C. Wu
Materialia 6 (2019) 100332.
ᅛయ㟁ゎ㉁䜢⏝䛔䛯㉳㟁ຊἲ䛻䜘䜛㧗 ⁐⼥ሷ䛾⇕ຊᏛ㔞䛾 ᐃ/
Measurement of Thermodynamic Properties in Molten Salts by EMF Method Using a Solid Electrolyte㛵ᮏ ⱥᘯ/ H. Sekimoto⁐⼥ሷ䛚䜘䜃㧗 ໬Ꮫ/ Molten Salsts 62(2) (2019) 68-74. (in Japanese)A first-principles theoretical study on the potential thermoelectric properties of MgH2 and CaH2
Y. Wang, Y. Ohishi, K. Kurosaki and H. Muta
Materials Research Express 6䠄䠄5䠅(2019) 055510.
Nanostructured bulk Si for thermoelectrics synthesized by surface diffusion/sintering doping
S-a Tanusilp, N. Sadayori and K. Kurosaki
RSC Advances 9(27) (2019) 15496-15501.
Release Kinetics of Tritium Generation in Neutron Irradiated Biphasic Li2TiO3-Li4SiO4 Ceramic Breeder
Q.L. Zhou, A. Togari, M. Nakata, M.Z. Zhao, F. Sun, Q. Xu, Y. Oya
Journal of Nuclear Materials 522 (2019) 286-293.
Thermal Stability of Microstrcutures and Mechanical Properties in a Fe-Based Fe-Cr-Mn-Cu-Mo Multi-Component
Alloy
Z.H. Zhong, Q. Xu, K. Mori and M. Tokitani
Philosophical Magazine 99 (2019) 1515-1527.
ΰྜ䜰䝙䜸䞁ᒙ≧໬ྜ≀ Sr2CrFeAsO3−δ 䛾Ꮚ☢Ẽ┦ᅗ/Electronic and Magnetic Phase Diagram of Mixed Anion
Layered Compound Sr2CrFeAsO3−δᒣཱྀ㐨ኴ㑻, ⸨ᒸᘯᏕ, ኱ሯ㈗ྐ, ℩ᡞㄔ, ໭ᑿ┿ྖ, ⓗሙṇ᠇, ⚄ཎ㝧୍/
M. Yamaguchi, H. Fujioka, T. Otsuka, M. Seto, S. Kitao, M. Matoba and Y. Kamihara᪥ᮏ☢ẼᏛ఍ㄽᩥ≉㞟ྕ/Transaction of the Magnetics Society of Japan Special Issues 3(1) (2019) 28-33.
(in Japanese)
Fabrication and Thermoelectric Property of Bi0.88Sb0.12/InSb Eutectic Alloy by Melt Spinning and Spark Plasma
Sintering
N.M. Natashah, Y. Ohishi, K. Kurosaki and H. Muta
MATERIALS TRANSACTIONS 60(6) (2019) 1072-1077/.
Light emission from treated surfaces of poly (ethylene terephthalate)
H. Nakamura, T. Kamata, N. Sato and K. Mori
Review of Scientific Instruments 90(6) (2019) 063104.
Si-Based Materials for Thermoelectric Applications
S-a Tanusilp and K. Kurosaki
Materials 12 (2019) 1943.
Density and viscosity of liquid ZrO2 measured by aerodynamic levitation technique
T. Kondo, H. Muta, K. Kurosaki, F. Kargl, A. Yamaji, M. Furuya and Y. Ohishi
Heliyon 7 (2019) e02049.

‑302‑

Crystal structure and hydrogen absorption- desorption property of La5Co19
K. Iwase, T. Ueno and K. MoriInternational Journal of Hydrogen Energy 44(41) (2019) 23172-23178.
Direct observation of interlayer molecular translational motion in a smectic phase and determination of the layerorder parameter
M. Saito, J. Yamamoto, R. Masuda, M. Kurokuzu, Y. Onodera, Y. Yoda and M. Seto
Physical Review Research 1 (2019) 012008.
First-principles calculation study of Mg2XH2 (X=Fe, Ru) on thermoelectric properties
Y. Wang, Y. Ohishi, K. Kurosaki and H. Muta
Materials Research Express 8 (2019) 085536.
Magnetic Field Induced Triple-q Magnetic Order in Trillium Lattice Antiferromagnet EuPtSi Studied by Resonant
X-ray Scattering
C. Tabata,T. Matsumura, H. Nakao, S. Michimura, M. Kakihana, T. Inami, K. Kaneko, M. Hedo, T. Nakama and Y.
ŌnukiJournal of the Physical Society of Japan 88(9) (2019) 093704.
Newly developed Laboratory-based Size exclusion chromatography Small-angle x-ray scattering System (La-SSS)
R. Inoue, T. Nakagawa, K. Morishima, N. Sato, A. Okuda, R. Urade, R. Yogo, S. Yanaka, M. Yagi-Utsumi, K. Kato,
K. Omoto, K. Ito and M. Sugiyama
Scientific Reports 9(1) (2019) 12610.
Time response of poly (ethylene naphthalate) light emission to charged particles
H. Nakamura and K. Mori
Physica Scripta 94(10) (2019) 105302.
125

Te-Mössbauer study of Fe1.1Te and FeTe0.5Se0.5 superconductor
S. Kitao, M. Kurokuzu, Y. Kobayashi and M. Seto
Hyperfine Interactions 240(1) (2019) 112.

Development of a measurement system enabling the reconstruction of γ-ray time spectra by simultaneous recordingof energy and time information
H. Tajima, S. Kitao, R. Masuda, Y. Kobayashi, T. Masuda, K. Yoshimura and M. Seto
Japanese Journal of Applied Physics 58(10) (2019) 108001.
The First Observation of Pure Nuclear Bragg Reflection from Natural Iron α-Fe2O3 by Synchrotron Mössbauer
Diffraction
S. Nakamura, T. Mitsui, Y. Kobayashi and S. Shimomura
Journal of the Physical Society of Japan 88(10) (2019) 103702.
A new and practical Se(IV) removal method using Fe3+ type cation exchange resin
D. Kawamoto, Y. Yamanishi, H. Ohashi, K. Yonezu, T. Honma, T. Sugiyama, Y. Kobayashi, Y. Okaue, A. Miyazaki
and T. Yokoyama
Journal of Hazardous Materials 378 (2019) 120593.
Thermophysical and mechanical properties of CrB and FeB
Y. Ohishi, M. Sugizaki, Y. Sun, H. Muta and K. Kurosaki
Journal of Nuclear Science and Technology 56(9-10) (2019) 859-865.
Design of S–S bond containing maleimide-conjugated closo-dodecaborate (SSMID): identification of uniquemodification sites on albumin and investigation of intracellular uptake
S. Ishii, S. Sato, H. Asami, T. Hasegawa, J. Y. Kohno and H. Nakamura
Organic & Biomolecular Chemistry 17 (2019) 5496-5499.
Dynamic motion and freezing of polaronic local structures in a colossal-magnetoresistive perovskitemanganite
La0.7Ca0.3MnO3 detected with radioactive nuclei
W. Sato, S. Komatsuda, H. Shimizu, R. Moriichi, S. Abe, S. Watanabe, S. Komatsu, T. Terai, S. Kawata and Y.
OhkuboPhysical Review B100 (2019) 184111.

‑303‑

Mössbauer Spectroscopy Study of KxFe2−ySe2 under Pressure
Y. Yamamoto, T. Mitsui, S. Kitao, M. Seto, N. Mizobata, T. Ozaki, H. Yamaoka and J. Mizuki
Journal of the Physical Society of Japan 12 (2019) 124703.
Positive Weiss Temperature in Layered Antiferromagnetic FeNiN for High-Performance Permanent Magnets ACS
S. Goto, H. Kura, H. Yanagihara, E. Kita, M. Tsujikawa, R. Sasaki, M. Shirai,Y. Kobayashi,T. Honda and K. Ono
Applied Nano Materials 2(11) (2019) 6909-6917.
Positron annihilation study on the phase transition of thermally aged Fe-Cr binary alloys at 748K
R. Kasada and K. Sato
Philosophical Magazine Letters 99(10) (2019) 360-371.
Thermal and mechanical properties of U3Si and USi3
A. Mohamad, W. Silpawilawan, H. Muta, K. Kurosaki and Y. Ohishi
Annals of Nuclear Energy 133 (2019) 186-193.
Effect of Annealing on the Microstructure Behavior of D+-Irradiated W-2vol.%TiC Composite Prepared by WetChemical Method
Y.X. Zhang, X.Y. Tan, X. Zan, L.M. Luo, Y. Xu, Q. Xu, K. Tokunaga, X.Y. Zhu and Y.C. Wu
Fusion Engineering and Design 148 (2019) 111321.
Effect of Interaction between H and He on Micro-Defects in Fe9Cr Alloy Investigated by Slow Positron Beam
L. Li, S.X. Jin, P. Zhang, D.D. Wang, X.Z. Cao, L.P. Guo, Q. Xu, J. Li, T.M. Zhang, L.B. Li, B.Y. Wang
Journal of Nuclear Materials 526 (2019) 15174.
Microscopic molecular translational dynamics in cholesteric and cholesteric blue phases
M. Saito, J. Yamamoto, R. Masuda, M. Kurokuzu, Y. Yoda and M. Seto
Hyperfine Interactions 241(1) (2019) 14.
Microstructural Evolution in W-1%TiC Alloy Irradiated He ions at High Temperatures
Q. Xu, H.Y. Chen, L.M. Luo, M. Miyamoto, M. Tokitani and Y.C. Wu
Tungsten 1 (2019) 229-235.
Microstructure Evolution of the W-TiC Composite Conducted by Dual-Effects from Thermal Shock and He-Ion Irradiation
Y.F. Zhou, X.Y. Tan, L.M. Luo, Y. Xu, X. Zan, Q. Xu, K. Tokunaga, X.Y. Zhu and Y.C. Wu
Tungsten 1 (2019) 213-219.
Negative ionic states of tin in the oxide superconductor Sr3−xSnO revealed by Mössbauer spectroscopy
A. Ikeda, S. Koibuchi, S. Kitao, M. Oudah, S. Yonezawa, M. Seto and Y. Maeno
Physical Review B 100(24) (2019) 245145.
Neutron Transmission Spectrum of Liquid Lead Bismuth Eutectic
Y. Oba, D. Ito, Y. Saito, Y. Onodera, J. D. Parker, T. Shinohara and K. Oikawa
Materials Research Proceedings 15 (2019) 160-164.
Origin of the mixed alkali effect in silicate glass
Y. Onodera, Y. Takimoto, H. Hijiya, T. Taniguchi, S. Urata, S. Inaba, S. Fujita, I Obayashi, Y. Hiraoka and S.
KoharaNPG Asia Materials 11(1) (2019) 75.
Simulation for the correlation of positron annihilation rate with charge density near defects in iron
L. Xiaoshuang, L. Xiangyu, W. Baoyi, L. Eryang, J. Shuoxue, Z. Yujie, Z.Te, C. Xingzhong, C. Guodong and Q. Xu
Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms
461 (2019) 88-92.
Slow-positron beamline temperature rise reduction at Kyoto University Research Reactor
A. Yabuuchi, R. Naka, K. Sato, Q. Xu and A. Kinomura
Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms
461 (2019) 137-141.
Swamps of Hydrogen in Equiatomic FeCuCrMnMo Alloys: First-Principles Calculations
X. L. Ren, P. H. Shi, W. W. Zhang, X. Y. Wu, Q. Xu and Y. X. Wang
Acta Materialia 180 (2019) 189-198.

‑304‑

Synchrotron-radiation-based Mössbauer absorption spectroscopy with high resonant energy nuclides
R. Masuda, K. Kusada, T. Yoshida, S. Michimura, Y. Kobayashi, S. Kitao, H. Tajima, T. Mitsui, H. Kobayashi, H.
Kitagawa and M. Seto
Hyperfine Interactions 240(1) (2019) 120.
Understanding diffraction patterns of glassy, liquid and amorphous materials via persistent homology analyses
Y. Onodera, S. Kohara, S. Tahara, A. Masuno, H. Inoue, M. Shiga, A. Hirata, K. Tsuchiya, Y. Hiraoka, I. Obayashi,
K. Ohara, A. Mizuno and O. Sakata
Journal of the Ceramic Society of Japan 127 (2019) 853-863.
Chemical Environment and Magnetic Moment Effects on Point Defect Formation in CoCrNi-Based Concentrated
Solid-Solution Alloys
H.Q. Guan, S.S. Huang, J.H. Ding, F.Y. Tian, Q. Xu and J.J. Zhao
Acta Materialia 187 (2020) 122-134.
Contribution of cadmium to the total amount of positron creation in a reactor-based slow positron beamline
A. Yabuuchi, T. Yoshiie and A. Kinomura
Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms
463 (2020) 40-49.
Influence of Helium Ion Irradiation Damage Behavior after Laser Tnermal Shock of W-2%Vol Y2O3 Composites
G. Yao, X.Y. Tan, L.M. Luo, X. Zan, Y. Xu, Q. Xu, X.Y. Zhu, K. Tokunaga and Y.C. Wu
Progress in Nuclear Energy 121 (2020) 103241.
Significant growth of vacancy-type defects by post-irradiation annealing in neon ion-irradiated tungsten probed by aslow positron beam
A. Yabuuchi, M. Tanaka and A. Kinomura
Journal of Nuclear Materials 531 (2020) 152018-1_152018-5.
Vacancy formation enthalpy in CoCrFeMnNi high-entropy alloy
K. Sugita, N. Matsuoka, M. Mizuno and H. Araki
Scripta Materialia 176 (2020) 32-35.
Deuterium irradiation resistance and relevant mechanism in W䇵ZrC/Sc2O3 composites prepared by spark plasma
sintering
G. Yao, H.Y. Chen, M.Q. Fu, L.M. Luo, X. Zan, Q. Xu, K. Tokunaga, X.Y. Zhu and Y.C. Wu
Progress in Nuclear Energy 120 (2020) 103215.
Evolution of Defects with Isochronal Annealing in Helium-Irradiated 316L Studied by Slow Positron Beam
L.G. Song, B.Y. Wang, T. Zhu, Y.H. Gong, Q. Xu, L.P. Guo, S.X. Jin, P. Zhang, Y.M. Song and X.Z. Cao
Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms
467 (2020) 80-85.
A Power Metallurgy Route to Fabricate CNT-Reinforced Molybdenum-Hafnium-Carbon Composites
Y. Wei, L.M. Luo, H.B. Liu, X. Zan, J.P. Song, Q. Xu, X.Y. Zhu and Y.C. Wu
Materials & Design 190 (2020) 108635.
Crystal structure, microhardness, and toughness of biomineral CaCO3
K. Iwase and K. Mori
Crystal Growth & Design 20(3) (2020) 2091-2098.
Effect of C on the Formation of Cu Precipitates and Vacancy Clusters in Neutron-Irradiated Fe-Cu Alloys
S. Huang and Q. Xu
Journal of Nuclear Materials 533 (2020) 152085.
Transport Parameters and Permeation Behavior of Hydrogen Isotopes in the First Wall Materials of Future Fusion
Reactors
Y. Xu, Z.S. Wu, L.M. Luo, X. Zan, X.Y. Zhu, Q. Xu and Y.C. Wu
Fusion Engineering and Design 155 (2020) 111563.
Proceedings
Effect of gamma irradiation dose on radiation damage in polystyrene and fused quartz
S. Konishi, H. Minagawa, S. Nakagawa, Q. Xu, and H. Tsuchida
Proceedings of 4th Japan-China Joint Workshop on Positron Science Nara, Japan (Oct.28-Nov.2, 2019).

‑305‑

Development of AMOC measurement system for radiation damage in materials under ion irradiation
H. Minagawa, S. Konishi, S. Nakagawa and H. Tsuchida
Proceedings of 4th Japan-China Joint Workshop on Positron Science Nara, Japan (Oct.28-Nov.2, 2019).
Vacancy migration behavior in a CoCrFeMnNi high entropy alloy
K. Sugita, R. Ogawa, M. Mizuno, H. Araki, A. Yabuuchi and A. Kinomura
MATERIALS RESEARCH MEETING 2019 Yokohama, Japan (Oct.10-14, 2019).
Irradiation-induced vacancy defects and its recovery behavior in 5N-purity tungsten and 3N-purity tantalum
M. Tanaka, A. Yabuuchi and A. Kinomura
18th International Conference on Positron Annihilation (ICPA-18) Orlando, USA (Dec.27, 2019)
050014-1_050014-4.
Magnetic Doppler broadening measurement on Gadolinium-doped GaN
M. Maekawa, S. Sakai, S. Hagiwara, A. Miyashita, K. Wada, A. Kawasuso, A. Yabuuchi and S. Hasegawa
18th International Conference on Positron Annihilation (ICPA-18) Orlando, USA (Dec.27, 2019)050007-1_050007-4.
⢏Ꮚ⥺↷ᑕ䛥䜜䛯໬ྜ≀ྜ㔠୰䛾Ḟ㝗䛻䜘䜛Ỉ⣲ᤕ⋓/Hydrogen trapping behavior at defects introduced by irradiation into compound alloys
F. Hori, A. Takano, K. Sugita, Y. Sumikura, Q. Xu and K. Ohsawa
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 26. (in Japanese)୰ᛶᏊᨺᑕ໬ศᯒἲ䛻䜘䜛ᒾ⤮ල䛻ྵ䜎䜜䜛ᚤ㔞ඖ⣲ศᯒ/
Analysis of trace elements in natural mineral pigments by instrumental neutron activation analysis
N. Hagura, Y. Okada, T. Uchiyama and Y. Minai
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 29. (in Japanese)䜲䜸䞁⃰ᗘㄪᩚ䛻䜘䜛䃒⥺↷ᑕ㑏ඖ Cu ⣔ྜ㔠䝘䝜⢏Ꮚ䛾ྜᡂไᚚ /Synthesis of Cu base alloy nanoparticles by gamma-ray irradiation reduction with various ion concentration ratio
Y. Uchimura, S. Toda, T. Yamada, T. Matsui, Q. Xu and F. Hori
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 35. (in Japanese)䝆䝹䝁䝙䜴䝮䛸䝖䝷䞁䝇䝣䜵䝸䞁䛾㘒⏕ᡂ䛻㛵䛩䜛◊✲ /Study on complexation of zirconium and transferrin
T. Suzuki, T. Kobayashi and T. Sasaki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 36. (in Japanese)䜺䞁䝬⥺⎔ቃୗ䛾ఏ㏦⥺㊰䛻䛚䛔䛶⏕ᡂ䛩䜛ບ㉳㟁ὶ䛾ホ౯/Estimation of the current generated in cables under gamma-ray irradiation
Y. Gotoh, Y. Okuno, N. Sato, M. Akiyoshi, M. Imaizumi, T. Kobayashi and T. Okamoto
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 50. (in Japanese)
Positron Annihilation Spectroscopy Characterization of Formation of Helium/Hydrogen-Vacancy Nano-Clusters in
FeCr Alloy
T. Zhu, B.Y. Wang, X.N. Lian, S.X. Jin, R.S. Yu, X.Z. Cao and Q. Xu
Proceeding of the 15th Workshop on Slow Positron Beam Techniques and Applications (Sept.2-6, 2019) 235-237.
Reviews䝬䝹䝏䜻䝱䝢䝷䝸䞊X ⥺䝺䞁䝈䜢⏝䛔䛯㢧ᚤ䝯䝇䝞䜴䜰䞊ศග/
Mössbauer microspectrometer with a multicapillary X-ray lens⠛⏣ ᆂྖ, ᑠᯘ ᗣᾈ/
K. Shinoda and Y. Kobayashiᒾ▼㖔≀⛉Ꮫ/Japanese Magazine of Mineralogical and Petrological Sciences 47(4) (2019) 163-167. (in Japanese)㔞Ꮚ䝡䞊䝮ᐇ㦂䛸ᵓ㐀䝰䝕䝸䞁䜾䛻䜘䜛ள㖄䝸䞁㓟ሷ䜺䝷䝇䛾⇕⭾ᙇಀᩘ␗ᖖ䛾㉳※䛾ゎ᫂ᑠ㔝ᑎ㝧ᖹ, ᑠཎ┿ྖ, ṇ஭༤࿴ᨺᑕග 32 (2019) 67-74. (in Japanese)‑306‑ΰྜ䜰䝙䜸䞁ᒙ≧໬ྜ≀ Sr2CrFeAsO3−δ 䛾㟁Ꮚ☢Ẽ┦ᅗ/Electronic and Magnetic Phase Diagram of Mixed Anion Layered Compound Sr2CrFeAsO3−δ᪥ᮏ☢ẼᏛ఍ㄽᩥ≉㞟ྕ/ᒣཱྀ 㐨ኴ㑻, ⸨ᒸ ᘯᏕ, ኱ሯ ㈗ྐ, ℩ᡞ ㄔ, ໭ᑿ ┿ྖ, ⓗሙ ṇ᠇, ⚄ཎ 㝧୍/Transaction of the Magnetics Society of Japan Special Issues 3(1) (2019) 28-33. (in Japanese)
Synchrotron Radiation-Based Quasi-Elastic Scattering Using Mössbauer Gamma Ray with neV-Energy Resolution
M. Saito, T. Kanaya and R. Mashita
High-Resolution Inelastic X-Ray Scattering [Working Title] (2019).
Books㘒య໬ྜ≀஦඾
኱ᕝᑦኈ,ᾏᓮ⣧⏨,㰻⸨ኴ㑻,బ䚻ᮌ㝧୍,୰ᮧ㻌 ᫭,᐀ീ㻌 ᝴,ᒣෆ㻌 ⬶,⬥⏣ஂఙ㘒య໬Ꮫ఍㻌
ᮅ಴ฟ∧ (2019). (in Japanese)ᇶ♏㧗ศᏊ⛉Ꮫ஭ୖ೔ኴ㑻㧗ศᏊᏛ఍ᮾி໬Ꮫྠே(2020). (in Japanese)
Other
Hydrogen trapping of defects introduced by irradiation in intermetallics
F. Hori, Y. Sumikura, K. Sugita, A. Takano, A. Iwase, M. Maekawa, A. Kawasuso, Q. Xu and K. Ohsawa
QST Takasaki Annual Report 2018 QST-M-23 (2020) 39.
Synthesis of Au stabilized Cu nanoparticles by gamma-ray irradiation reduction method
F. Hori, Y. Uchimura, S. Toda, T. Matsui, A. Iwase, N. Taguchi, S. Tanaka and Q. Xu
Photon Factory Activity Report 2018 (2019) 36-39.
ᚋ⸨ᗣோ,ዟ㔝Ὀᕼ,బ⸨ಙᾈ,⛅ྜྷඃྐ,௒Ἠ㻌 ඘,ᑠᯘ▱ὒ,ᒸᮏ㻌 ಖᨺᑕ⥺⎔ቃୗ䛾䝉䞁䝃ฟຊ䜢ఏ㏦䛩䜛⥺㊰䛻䛚䛔䛶⏕ᡂ䛩䜛䜺䞁䝬⥺ບ㉳㟁ὶ䛾ホ౯㟁Ꮚ᝟ሗ㏻ಙᏛ఍ ᢏ⾡◊✲ሗ࿌ 119(305) (2019) 39-42. (in Japanese)

5. Geochemistry and Environmental Science
Papers
EFFECT ON MICROBIAL PRODUCTS ON CAESIUM ELUTION BEHAVIOUR FROM CLAY MINERALS
T. Kimura, S. Fukutani, K. Yamaji, M. Ikegami and M. Yoneda
Radiation Protection Dosimetry 184(3-4) (2019) 385-387.
Gastrointestinal Absorption Rate in Rats for Radiocesium in Soil Collected near Fukushima Power Plant or Doped
Artificially with 134CsCl
K. Iwata, T. Takahashi, S. Tanaka, T. Kubota, S. Fukutani, Y. Kinashi, M. Konno, Mitsuyuki,S. Mizuno and S.
Takahashi
Japanese Journal of Health Physics 54(1) (2019) 66-71.
Scaling Relationships of Source Parameters of Inland Crustal Earthquakes in Tectonically Active Regions
K. Miyakoshi, K. Somei, K. Yoshida, S. Kurahashi, K. Irikura and K. Kamae
Pure and Applied Geophysics 1 (2019) 13.
Vertical Migration of 137Cs in Japanese Orchards after the Fukushima Daiichi Nuclear Power Plant Accident
M. Sato, K. Matsuoka, T. Takase, N.I. Kobayashi, H. Kikunaga, D. Takata, K. Tanoi, T. Ohtsuki, S. Kusaba andK. Yamaguchi
The Horticulture Journal 88 (2) (2019) 150-163.
Y. Ohtsuka, M. Aoyama, Y. Takaku, Y. Igarashi, M. Hattori, K. Hirose and S. Hisamatsu
Pu/239Pu and 242Pu/239Pu atom ratios of Japanese monthly atmospheric deposition samples during 1963–1966
Scientific Reports 9(1) (2019) 8105.

240

‑307‑

Correlation between Different Type of Caesium Carrier in The Radiocaesium Interception Potential Measurementfor Forest Soils
H.A Pratama, M. Yoneda, Y. Shimada, S. Fukutani and M. Ikegami
Journal of Physics: Conference Series 1198(2) (2019) 022026.
Aerosol mixing state revealed by transmission electron microscopy pertaining to cloud formation and human airway
deposition
J. Ching, K. Adachi, Y. Zaizen, Y. Igarashi and M. Kajino
npj Climate and Atmospheric Science 2 (2019) 22.
ேᕤᵓ㐀≀࿘㎶䛾ᆅୗỈὶືཬ䜃Ỉ㉁ኚືゎᯒ㇂ཱྀᩥ⣖, ⸨ᕝ㝧Ꮚ, ᅜศᏹᇛ, ᶫᮏⰾ, ᮧἑ┤἞, ᑿᓮ༤᫂➨ 25 ᅇᆅୗỈ㽂ᅵተởᰁ䛸䛭䛾㜵Ṇᑐ⟇䛻㛵䛩䜛◊✲㞟఍ㅮ₇㞟 25 (2019) 455-459. (in Japanese)ᆅୗỈ୰䛾ᨺᑕᛶ䝉䝅䜴䝮䞊⚟ᓥ┴὾㏻䜚,୰㏻䜚䛚䜘䜃఍ὠ䛷䛾ㄪᰝ⤖ᯝ⸨ᕝ㝧Ꮚ, ㇂ཱྀᩥ⣖, ᅜศᏹᇛ, ᶫᮏⰾ, ᮧἑ┤἞, 㟼㛫Ύ➨ 25 ᅇᆅୗỈ㽂ᅵተởᰁ䛸䛭䛾㜵Ṇᑐ⟇䛻㛵䛩䜛◊✲㞟఍ㅮ₇㞟 25 (2019) 408-412. (in Japanese)᣺ືィ 䛻ᇶ䛵䛟ഴᩳᇶ┙ୖ䛻ᘓ䛴ච㟈ᘓ≀䛾᣺ືᛶ≧䛻㛵䛩䜛᳨ウ/
Dynamic Properties of a Seismically-Isolated Building Constructed on Soil with Inclined Bedrock from Vibration
Measurementsすᾆ 㑈, Ọ㔝ṇ⾜, 㣕⏣႐๎, ୖᯘᏹᩄ/R. Nishimura, M. Nagano, Y. Tobita and H. Uebayashi᪥ᮏᆅ㟈ᕤᏛ఍ㄽᩥ㞟/
Journal of Japan Association for Earthquake Engineering 19(6) (2019) 181-192. (in Japanese)⚟ᓥ➨୍ཎᏊຊⓎ㟁ᡤ஦ᨾ䛻䜘䜚 1 ྕᶵ䛛䜙ᨺฟ䛥䜜䛯ᨺᑕᛶ䜶䜰䝻䝌䝹䛾≀⌮䞉໬Ꮫⓗᛶ≧䛾ゎ᫂/Investigation of Physical and Chemical Characteristics of Radioactive Aerosols Emitted From Reactor Unit 1 by
Fukushima Daiichi Nuclear Power Plant Accident
S. Onozaki, Y. Abe, I. Nakai, K. Adachi, Y. Igarashi, Y. Oura, M. Ebihara, T. Miyasaka, H. Nakamura, K. Sueki, H.
Tsuruta and Y. Moriguchi
BUNSEKI KAGAKU 68(10) (2019) 757-768. (in Japanese)
S. Yokoyama, T. Takahashi, M. Ota, H. Kakiuchi, S. Sugihara, S. Hirano, N. Momoshima, T. Tamari, N. Shima, M.
Atarashi-Andoh, S. Fukutani, S. Nakasone, M. Furukawa, M. Tanaka and N. Akata
Development of Field Estimation Technique and Improvement of Environmental Tritium Behavior Model
Plasma and Fusion Research 14 (2019) 3405099-1_3405099-4.
Petit-spot volcanoes on the oldest portion of the Pacific plate
N. Hirano, S. Machida, H. Sumino, K. Shimizu, A. Tamura, T. Morishita, H. Iwano, S. Sakata, T. Ishii, S. Arai, S.
Yoneda, T. Danhara and T. Hirata
Deep Sea Research Part I: Oceanographic Research Papers 159 (2019) 103142.
Tritium separation from heavy water using a membrane containing deuterated manganese dioxide
H. Koyanaka, S. Fukutani and H. Miyatake
Radioanalytical and Nuclear Chemistry 322(3) (2019) 1889-1895.

Journal ofᨺᑕᛶ᰾✀䛾኱Ẽᨺฟ䛸኱Ẽ୰ືែ䛾⌮ゎ䛾⌧≧/
Recent Understanding on the Release of Radionuclides and Their Behavior in the Atmosphereᒣ⃝ᘯᐇ䠈஬༑ᔒᗣே/H. Yamazawa and Y. Igarashi
RADIOISOTOPES 69 (2019) 19-30. (in Japanese)
Proceedings
Petit-spot and seamount rejuvenation overprinting western Pacific plate
N. Hirano and H. Sumino
AGU Fall Meeting 2019 San Francisco, California, USA (Dec.9-13, 2019) V11E-0142.
Performance of a 500 L SNAP reactor placed in the downstream of biological filtration system for removal of arsenicfrom groundwater
Y. Fujikawa, Ph. D. Hung, D. Hira, T. Fujii, H. Ozaki and K. Furukawa
Proceedings of 4th International Symposium IANAS2019 Osaka, Japan (Nov.13-15, 2019) 226-231.

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Microbiome analysis of samples from a single stage partial nitritation - anammox reactor used for treatment ofgroundwater
Y. Fujikawa, D. Hira, I. Suzuki, Ph. D. Hung, T. Fujii, K. Kokubun and K. Furukawa,
Proceedings of 4th International Symposium IANAS2019 Osaka, Japan (Nov.13-15, 2019) 274-279.
⚟ᓥཎⓎ஦ᨾ䛷ᨺฟ䛥䜜䛯ᨺᑕᛶᚤ⢏Ꮚ䛾ศᯒ䛚䜘䜃ᶍᨃ⏕ᡂᐇ㦂/
Analysis and simulated generation
experiment for radioactive particles released by the Fukushima nuclear accident
Makoto Inagaki, Ryo Sato, Shun Sekimoto, Koichi Takamiya, Yuichi Oki, Tsutomu Ohtsuki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 30. (in Japanese)᰾ศ⿣⏕ᡂ≀䛸⁐ᾮ䜶䜰䝻䝌䝹⢏Ꮚ䛾㟼㟁┦஫స⏝䛻䜘䜛྾╔ᣲື/
Attachment behavior of fission products on solution aerosol by electrostatic interaction
Y. Takeuchi, T. Takeuchi, K. Takamiya, M. Inagaki, S. Sekimoto, Y. Oki and T. Ohtsuki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 53. (in Japanese)᰾ศ⿣⏕ᡂ≀䛸⁐ᾮ䜶䜰䝻䝌䝹⢏Ꮚ䛾㟼㟁┦஫స⏝䛻䜘䜛྾╔ᣲື/
Attachment behavior of fission products on solution aerosol by electrostatic interaction
T. Takeuchi, Y. Takeuchi, K. Takamiya, M. Inagaki, S. Sekimoto, Y. Oki and T. Ohtsuki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 54. (in Japanese)ᨺᑕᛶ≀㉁䛾኱Ẽỿ╔䞉ᣑᩓ䛚䜘䜃㝣ᇦ䛛䜙䛾෌ᾋ㐟䛻䛴䛔䛶/
Atmospheric deposition and diffusion of radioactive materials from the F1NPP accident and their resuspension
Y. Igarashi
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 71-73. (in Japanese)
Reviews
Accurate determination of three halogen elements (Cl, Br, and I)in U.S. Geological Survey geochemical referencematerials by radiochemicalneutron activation analysis and an exhaustive comparison with literaturedata: a review
S. Sekimoto and M. Ebihara
Journal of Nuclear and Radiochemical Science 20 (2020) 12-19.
ᒣ⃝ᘯᐇ䠈஬༑ᔒᗣே/H. Yamazawa and Y. Igarashiᨺᑕᛶ᰾✀䛾኱Ẽᨺฟ䛸኱Ẽ୰ືែ䛾⌮ゎ䛾⌧≧/
Recent Understanding on the Release of Radionuclides and Their Behavior in the Atmosphere
RADIOISOTOPES 69(1) (2019) 19-30. (in Japanese)ᮌᮧᘓ㈗, ⚟㇂ ဴ, ᒣ㊰ ᜨᏊ, ụୖ 㯞⾰Ꮚ/
T. Kimura, S. Fukutani, K. Yamaji and M. Ikegami䝅䝕䝻䝩䜰䛻䜘䜛⢓ᅵ㖔≀୰䝉䝅䜴䝮䛾⬺㞳⌧㇟䛻㛵䛩䜛◊✲/A STUDY OF CESIUM ELUTION BEHAVIOR FROM CLAY MINERALS TRIGGERED BY SIDEROPHORESᅵᮌᏛ఍ㄽᩥ㞟 G䠄⎔ቃ䠅/Journal of Japan Society of Civil Engineers, Ser. G (Environmental Research) 7 (2019) 503-508. (in Japanese)
A review of Cs-bearing microparticles in the environment emitted by the Fukushima Dai-ichi Nuclear Power Plant
accident
Y. Igarashi, T. Kogure, Y. Kurihara, H. Miura, T. Okumura, Y. Satou, Y. Takahashi and N. Yamaguchi
Journal of Environmental Radioactivity 205-206 (2019) 101-118.
Books
Environmental Contamination from the Fukushima Nuclear Disaster
Part I. Dynamics of Radioactive Materials in the Environment:1. Introduction 䇵 basic concepts regarding the
Fukushima accident, radiation and radioactivity
T. Nakajima, T. Ohara, M. Uematsu, Y. Onda, M. Ebihara, A. Shinohara, Y. Hamajima, Y. Igarashi, T. Aono,
M. Aoyama, M. Takigawa and K. Saito, T. Nakajima, T. Ohara, M. Uematsu and Y. Onda
Cambridge University Press (2019).

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኱Ẽ⎔ቃ䛾஦඾
ཎⓎ஦ᨾ䛻䜘䜛⎔ቃᙳ㡪஬༑ᔒᗣே኱Ẽ⎔ቃᏛ఍ 䠄⦅䠅ᮅ಴᭩ᗑ(2019). (in Japanese)

6. Life Science and Medical Science
PapersCatalytic Hydrolysis of Phosphate Monoester by Supramolecular Phosphatases Formed from a Monoalkylated
Dizinc(II) Complex, Cyclic Diimide Units, and Copper(II) in Two-Phase Solvent System
A.B Rahman, H. Imafuku, Y. Miyazawa, A. Kafle, H. Sakai, Y. Saga and S. Aoki
Inorganic Chemistry 58(9) (2019) 5603-5616.
Structural Insights into the Inhibition of Amyloid Fibril Formation by Fibrinogen via Interaction with Prefibrillar
N. Yamamotoi, T. Akai, R. Inoue, M. Sugiyama, A. Tamura and E. ChataniIntermediates Biochemistry 58(24) (2019) 2769-2781.
Structural characterization of the N-terminal kinase-interacting domain of an Hsp90-cochaperone Cdc37 by CD andsolution NMR spectroscopy
F. Ihama, M. Yamamoto, C. Kojima, T. Fujiwara, K. Matsuzaki, Y. Miyata and M. Hoshino
Biochimica et Biophysica Acta (BBA) - Proteins and Proteomics 1867(9) (2019) 813-820.
Catalytic Hydrolysis of Phosphate Monoester by Supramolecular Complexes Formed by the Self-Assembly of a
Hydrophobic Bis(Zn2+-cyclen) Complex, Copper, and Barbital Units That Are Functionalized with Amino Acids
in a Two-Phase Solvent System
Y. Miyazawa, A.B. Rahman, Y. Saga, H. Imafuku, Y. Hisamatsu and S. Aoki
Micromachines 710(7) (2019) 452.
Design, Synthesis, DNA/HSA Binding, and Cytotoxic Activity of Half-Sandwich Ru(II)-Arene Complexes
Containing Triarylamine–Thiosemicarbazone Hybrids
M. Muralisankar, R. Dheepika, J. Haribabu, C. Balachandran, S. Aoki, N.S.P. Bhuvanesh and S. Nagarajan
ACS Omega 4(7) (2019) 11712-11723.
Dynamic Views of the Fc Region of Immunoglobulin G Provided by Experimental and Computational Observations
S. Yanaka, R. Yogo, R. Inoue, M. Sugiyama, S.G. Itoh, H. Okumura, Y. Miyanoiri, H. Yagi, T. Satoh, T. Yamaguchi
and K. Kato.
Antibodies 8(3) (2019) 39.
NHC-catalyzed green synthesis of functionalized chromones: DFT mechanistic insights and in vitro activities incancer cells
N. Murugesh, J. Haribabu, K. Arumugam, C. Balachandran, R. Swaathy, S. Aoki, A. Sreekanth, R. Karvembu and
S. Vedachalam.
New Journal of Chemistry 43 (2019) 13509-13525.
Design, synthesis, and anticancer activity of iridium(III) complex-peptide hybrids that contain hydrophobic acylgroups at the N-terminus of the peptide units
K. Naito, K. Yokoi, C. Balachandran, Y. Hisamatsu and S. Aoki.
Journal of Inorganic Biochemistry 199 (2019) 110785.
A New Class of β–Pyrrolidino-1,2,3-Triazole Derivatives as β-Adrenergic Receptor Inhibitors: Synthesis,
Pharmacological, and Docking Studies
M. Easwaramoorthi, J.A Rajendran, K.C. Rao, C. Balachandran, Y. Arun, S.M. Mahalingam, N. Arumugam, A.
Almansour, R.S. Kumar, D.M. Al-thamili and S. Aoki
Molecules 24(19) (2019) 3501.
Cisplatin Facilitates Radiation-Induced Abscopal Effects in Conjunction with PD-1 Checkpoint Blockade Through
CXCR3/CXCL10-Mediated T-cell Recruitment
R. Luo, E. Firat, S. Gaedicke, E. Guffart, T. Watanabe and G. Niedermann
Clinical Cancer Research 23 (2019) 7243-7255.

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Purified F-ATP synthase forms a Ca2+-dependent high-conductance channel matching the mitochondrial
permeability transition pore
A. Urbani, V. Giorgio, A. Carrer, C. Franchin, G. Arrigoni, C. Jiko, K. Abe, S. Maeda, K. Shinzawa-Itoh, J.F.M.
Bogers, D.G.G McMillan, C. Gerle, I. Szabò and P. Bernardi
Nature Communications 1 (2019) 4341.
Crystal structure of pantoate kinase from Thermococcus kodakarensis
A. Kita, A. Kishimoto, T. Shimosaka, H. Tomita, Y. Yokooji, T. Imanaka, H. Atomi and K. Miki
Proteins: Structure, Function, and Bioinformatics 88(5) (2020) 718-724.
Regulation of plant ER oxidoreductin 1 (ERO1) activity for efficient oxidative protein folding
M. Matsusaki, A. Okuda, K. Matsuo, K. Gekko, T. Masuda, Y. Naruo, A. Hirose, K. Kono, Y. Tsuchi and R. Urade
Journal of Biological Chemistry 49 (2019) 18820-18835.
The design and green synthesis of novel benzotriazoloquinolinyl spirooxindolopyrrolizidines: antimycobacterial andantiproliferative studies
V. Pogaku, V.S. Krishna, C. Balachandran, K. Rangan, D. Sriram, S. Aoki and S. Basavoju
New Journal of Chemistry 44 (2019) 17511-17520.
Ubiquitin carboxyl䇲terminal hydrolase L1 promotes hypoxia䇲inducible factor 1䇲dependent tumor cell malignancy
in spheroid models
X. Li, A. Hattori, S. Takahashi, Y. Goto, H. Harada and H. Kakeya
Cancer Science 111 (2019) 239-252.
Increased 14C-acetate accumulation in IDH-mutated human glioblastoma: implications for detecting IDH-mutatedglioblastoma with 11C-acetate PET imaging
S. Koyasu, Y. Shimizu, A. Morinibu, T. Saga, Y. Nakamoto, K. Togashi and H. Harada
Journal of Neuro-Oncology 145(3) (2019) 441-447.
Structural Studies of Overlapping Dinucleosomes in Solution
A. Matsumoto, M. Sugiyama, Z. Li, A. Martel, L. Porcar, R. Inoue, D. Kato, A. Osakabe, H. Kurumizaka and H. Kono
Biophysical Journal 118(9) (2019) 2209-2219.
Adding Indoximod to Hypofractionated Radiotherapy with Anti-PD-1 Checkpoint Blockade Enhances Early NK
and CD8+ T-Cell䇵Dependent Tumor Activity
T. Watanabe, S. Gaedicke, E. Guffart, E. Firat and G. Niedermann
Clinical Cancer Research 26(4) (2020) 945-956.
One-pot synthesis of cyclic oligosaccharides by the polyglycosylation of monothioglycosides
H. Someya, T. Seki, G. Ishigami, T. Itoh, Y. Saga, Y. Yamada and S. Aoki
Carbohydrate Research 487 (2020) 107888.
Supramolecular tholos-like architecture constituted by archaeal proteins without functional annotation
M. Yagi-Utsumi, A. Sikdar, C. Song, J. Park, R. Inoue, H. Watanabe, R.N. Burton-Smith, T. Kozai, T. Suzuki, A.
Kodama, K. Ishii, H. Yagi, T. Satoh, S. Uchiyama, T. Uchihashi, K. Joo, J. Lee, M. Sugiyama, K. Murata and K.
Kato
Scientific Reports 10 (2020) 1540-1540.
Unprecedented formation of palladium(II)-pyrazole based thiourea from chromone thiosemicarbazone and[PdCl2(PPh3)2]: Interaction with biomolecules and apoptosis through mitochondrial signaling pathway
J. Haribabu, C. Balachandran, M.M. Tamizh, Y. Arun, N. S.P. Bhuvanesh, S. Aoki and R. Karvembu
Journal of Inorganic Biochemistry 205 (2020) 110988.
Current status and near future plan of neutron protein crystallography at J-PARC
I. Tanaka, T. Chatake, S. Fujiwara, T. Hosoya, K. Kusaka, N. Niimura, T. Yamada and N. Yano
Methods in Enzymology 634 (2020) 101-123.
Disturbance in the regulation of miR 17-92 cluster on HIF-1-α expression contributes to clinically relevantradioresistant cells: an in vitro study
M.H. Roudkenar, M. Fukumoto, A.M. Roushandeh, Y. Kuwahara, Y. Uroshihara, H. Harada and M. Fukumoto
Cytotechnology 20(1) (2020) 141-153.

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A single Asp isomer substitution in an αA-crystallin-derived peptide induces a large change in peptide properties
K. Magami, I. Kim and N. Fujii
Experimental Eye Research 192 (2020) 107930.
Proceedings
Development of a proton range-verification method using ionoacoustic waves generated from spherical metal
markers
T. Takayanagi,T. Uesaka, Y. Nakamura, M. B. Unlu, Y. Kuriyama, T. Uesugi, Y. Ishi, K. Umegaki, H. Shirato and
T. Matsuura
The 58th Annual Conference of the Particle Therapy Co-Operative Group (PTCOG58) Manchester, UK(June10-15, 2019).
Development of Glass-Beads Filters for the Isolation, Culture, and Re-collection of Cancer Cells
S. Aoki, B. Shashni, S. Ariyasu, H. Takemura, K. Akimoto, N. Aikawa, K. Iwasaki, T. Nakanishi, A. Yasumori,T. Osaki and N. Itoh
International e-Conference on Cancer Research 2019 (e-ICCR 2019) London, United Kingdom (June10-11, 2019).
CTCs extraction method based on frequency-domain filtering from microscope images
K. Yoshida, Y. J. Chen, L. S. Lu, S. Aoki, and N. Aikawa,
23rd IEEE International Conference on Signal Processing: Algorithms, Architectures, Arrangements, andApplications Poznan, Poland (Sept.18-20, 2019) 186-191.
Hydrogen/deuterium exchange behavior in tetragonal hen egg-white lysozyme crystals analyzed by the neutron
diffraction methods
A. Kita and Y. Morimoto
6th International Symposium on Diffraction Structure Biology Osaka, Japan (Oct.17-20, 2019).
Hydrogen/deuterium exchange behavior in tetragonal hen egg-white lysozyme crystals
A. Kita and Y. Morimoto
16th Conference of the Asian Crystallographic Association Singapore (Dec.17-20, 2019).
Structural analysis of ligand binding mechanism of L-lactate oxidase from Aerococcus viridans by use of ligand
soaking crystals
Y. Morimoto, N. Furubayashi, M. Kamo, Y. Umena, A. Kita, T. Matsuoka and K. Inaka
16th Conference of the Asian Crystallographic Association Singapore (Dec.17-20, 2019).
䝬䝹䝏䝗䝯䜲䞁䝍䞁䝟䜽㉁䛾䝁䞁䝖䝷䝇䝖ྠㄪ୰ᛶᏊᑠゅᩓ஘ゎᯒ䛾䛯䜑䛾䜻䝯䝷㔜Ỉ⣲໬䝍䞁䝟䜽㉁స〇ἲ䛾☜❧/
Establishing the method of chimera-deuterated protein synthesis for contrast-matching SANS
A. Okuda, K. Morishima, N. Sato, R. Inoue, R. Urade and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 21. (in Japanese)䜰䝭䝻䜲䝗᰾ᙧᡂ䝯䜹䝙䝈䝮䛾ゎ᫂䜢┠ᣦ䛧䛯᰾ᙧᡂ୰㛫య䛾ᤕᤊ䛸ᵓ㐀ゎᯒ/Trapping and structural analysis of nucleation intermediates aimed at clarifying amyloid nucleation mechanisms
Y. Yoshikawa, N. Yamamoto, R. Inoue, K. Morishima, M. Sugiyama, A. Tamura and E. Chatani
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 23. (in Japanese)䝬䝹䝏䝗䝯䜲䞁⺮ⓑ㉁䛾㝵ᒙⓗ䛺ືⓗᵓ㐀䛸䝎䜲䝘䝭䜽䝇/
Solution structure of multi-domain protein
H. Nakagawa, T. Saio, M. Sugiyama, R. Inoue, M. Nagao and T. Tominaga
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 24. (in Japanese)X ⥺ᑠゅᩓ஘䛻䜘䜛䜰䝭䝻䜲䝗⥺⥔๓㥑୰㛫యⓎ㐩䛾᫬ศ๭㏣㊧/Monitoring structural formation of amyloid prefibrillar intermediates by small-angle X-ray scattering
N. Yamamoto, T. Akai, R. Inoue, M. Sugiyama, N. Shibayama and E. Chatani
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 25. (in Japanese)ྂ⣽⳦䛾㞟ྜ䝅䝱䝨䝻䞁ᵝ䝍䞁䝟䜽㉁ PbaA 䛾ືⓗᵓ㐀ゎᯒ/
Dynamical structure of archaeal homolog of proteasome-assembly chaperone PbaA
M. Y. Utsumi, R. Inoue, M. Sugiyama and K. Kato
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 27. (in Japanese)‑312‑

Solution structure of the circadian clock protein complex characterized by a combination approach involving
solution scattering and computational methods
Y. Yunoki, H. Yagi, K. Morishima, J. Matsumoto, N. Sato, L. Porcar, A. Martel, R. Inoue,T. Kazuki, H. Kono,
K. Kato and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 28. (in Japanese)䝯䝍䞁⳦⏤᮶ sHsp 䛾 ᗘ౫Ꮡᛶᶵᵓ䛾ゎ᫂/
Study on the temperature dependency of sHsps from methanogens
M. Yohda, A. Kanno, R. Inoue, N. Sato, K. Morishima and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 37. (in Japanese)⁐ᾮ≧ែ䜢཯ᫎ䛧䛯,㔜Ỉ⣲໬䝍䞁䝟䜽㉁䛾୰ᛶᏊ⥺⤖ᬗᵓ㐀ゎᯒ/
Neutron crystallographic studies for deuterated protein that reflects the solvent state
A. Kita and Y. Morimoto
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 41. (in Japanese)ᾏ⸴⏤᮶䝣䝁䜲䝎䞁䛻䜘䜛䜰䝭䝻䜲䝗จ㞟ᢚไᶵᵓ䛾ゎᯒ/Inhibitory mechanism of amyloid fibril formation by sea-weed fucoidan
M. Hoshino, Y. Kato, K. Morishima, R. Inoue, M. Subiyama and H. Yagi
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 42. (in Japanese)ᑠゅᩓ஘ἲ䛸ศᯒ㉸㐲ᚰ䛻䜘䜛䝍䞁䝟䜽㉁⁐ᾮᩓ஘䛛䜙䛾จ㞟㝖ཤゎᯒ/Aggregation elimination analysis of protein solution scattering with small angle scattering and analyticalultracentrifugation
Y. Miyamoto, K. Morishima, R. Inoue, N. Sato, A. Okuda, R. Urade and M. Sugiyama
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 48. (in Japanese)᳜≀ᑠ⬊య䛷䛾᪂⏕䝍䞁䝟䜽㉁䛾㓟໬ⓗ䝣䜷䞊䝹䝕䜱䞁䜾ᶵᵓ/
Mechanism of oxidative folding in plant endoplasmic reticulum
R. Urade
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 61-63. (in Japanese)ఇṆᮇ⭘⒆⣽⬊≉ᛶ䛸⒴ᖿ⣽⬊ᛶ䛸䛾㛵㐃ᛶゎᯒ䛸⒴἞⒪䜈䛾ᛂ⏝ቑỌៅ୍㑻,┿⏣ᝆ⏕,⏣㔝ᜨ୕➨ 22 ᅇⳢཎ䞉኱すグᛕ⒴἞⒪ቑឤ䝅䞁䝫䝆䜴䝮 ዉⰋ(Feb.8-9, 2020). (in Japanese)
IDO inhibition strongly enhances effects of combined hRT and PD1/PD-L1 checkpoint blockade
T. Watanabe and G. Niedermann
Radiotherapy and Oncology Milan, Italy (Apr.26-30, 2019) S72-S73.
Indoximod Strongly Enhances Effects of Combined Hrt and PD1/PD-L1 Checkpoint Blockade
T. Watanabe and G. Niedermann
International Journal of Radiation Oncology, Biology, Physics Chicago, USA (Sept.15-19, 2020) E652.
Book䝍䞁䝟䜽㉁䛾䜰䝰䝹䝣䜯䝇จ㞟䛸⁐ゎᛶ䇷ᇶ♏◊✲䛛䜙䝞䜲䜸⏘ᴗ䞉๰⸆◊✲䜈䛾ᛂ⏝䜎䛷䇷㯮⏣㻌 ⿱, ᭷ᆏᩥ㞝, ⓑᮌ㈼ኴ㑻, ᒾୗ࿴㍤, ୕ᮧ┿኱, ᐀㻌 ṇᬛ, ᚋ⸨♸ඣ, ௒ᮧẚ࿅ᚿ, Ώ㑔⚽ᶞ, ༓㈡⏤ెᏊ, ᮏ⏣┿ஓ, ኴ⏣㔛Ꮚ, ᮡᒣṇ᫂, ᇛᡤಇ୍, ⱝᒣㄹ኱, ෆᒣ㻌 㐍 , 䝕䝭䜶䞁 䝩䞊䝹, ᘅ⏣ዉ⨾, ஬ᓥ┤ᶞ, Ἑᮧ⩏ྐ, ᘅ℩ಟ୍,㔝ཱྀ㻌 ಖ, ୹⩚㐩ஓ, ⏣ཱྀⱥᶞ, ఀ㇋ὠ೺୍, ὠᮏᾈᖹ, ఀ಴㈆ྜྷ, ụཱྀ㞞㐨, Ⲩᕝ㻌 ຊ, Ụᓥ
኱㍜, ὸ㔝❳ኴ㑻, ㉥⃝㝧Ꮚ, ⴗཎ⩏ஂ, ᑠ⃝኱స, Ṋෆᩄ⚽, Ọ஭⩏㝯, Ᏻ⸨᫛୍ᮁ, ▼ཎᬛᙪ,ᑠ㔝ᑎ㻌 ⌮ ,ຍ⸨ᫀே, ⡿⏣᪩⣖, 㫽ᕢဴ⏕, 㯮㇂⠜அ, ᰘ⏣ᐶᏊ, ▼஭᫂Ꮚ, 㯮⏣⿱, ᭷ᆏᩥ㞝➨䊡⦅ ➨ 4 ❶㻌 ᑠゅᩓ஘ἲ䠄ᰴ䠅䝅䞊䜶䝮䝅䞊ฟ∧ (2019). (in Japanese)
Reviewsᮡᒣ ṇ᫂, ஭ୖ ೔ኴ㑻, ୰ᕝ ὒ, 㰻ᑿ ᬛⱥ୰ᛶᏊ⁐ᾮᩓ஘ : ⌧ᅾ䞉㐣ཤ䞉ᮍ᮶(≉㞟 Ἴ⣠ห⾜ 30 ᖺグᛕ≉㞟 䛣䜜䛛䜙䛾୰ᛶᏊ⛉Ꮫ䝁䝭䝳䝙䝔䜱䛾ᅾ䜚᪉䛸䛿)Ἴ⣠ : Neutron network news 30(1) (2020) 16-25. (in Japanese)‑313‑ప㓟⣲䝞䜲䜸䝻䝆䞊䛾๰㐀䛸㐍ᒎཎ⏣ᾈᨺᑕ⥺⏕≀◊✲ 55(1) (2020) 61-67. (in Japanese)Ỉᬗయෆ䜽䝸䝇䝍䝸䞁୰䛾䜰䝇䝟䝷䜼䞁㓟ṧᇶ䛾␗ᛶ໬/The spontaneous isomerization of aspartate residues in lens crystallin㧗⏣໶, ⸨஭⣖Ꮚ/
T. Takata and N. Fujii⏕໬Ꮫ/
Journal of Japanese Biochemical Society 91(3) (2019) 322-328. (in Japanese)䛜䜣἞⒪䛻䛚䛡䜛 Particle Therapy 䛾⌧≧䛸ᒎᮃ▼ᕝோ, ୰஭ၨ, 㔝୰ဴ⏕, Ḉ஭ⱥᖾ⒴䛸໬Ꮫ⒪ἲ 46(8) (2019) 1219-1225. (in Japanese)䝠䝖Ỉᬗయຍ㱋䝰䝕䝹⺮ⓑ㉁䛾⇕Ᏻᐃᛶ䛸䝅䝱䝨䝻䞁ᵝᶵ⬟䛾 ᐃ㧗⏣໶, ⸨஭⣖Ꮚ
Jasco Report 61(2) (2019) 1-6. (in Japanese)䝇䝖䝺䝇ㄏⓎ⣽⬊⪁໬䛿⅖⑕䞉䛜䜣⣽⬊ቑṪಁ㐍䛻㛵୚䛩䜛/Stress-induced Cellular Senescence Contributes to Chronic Inflammation and Cancer Progression Thermalᑠᶫᕝ ᪂Ꮚ, ᆏཱྀ ⩏ᙪ, ቑỌ ៅ୍㑻, ᳃ ⱥ୍ᮁ/S. Kobashikawa, Y. M. SakaguchiI, S. Masunaga and E. Mori
Medicine 35(4) (2019) 41-58. (in Japanese)

7. Neutron Capture Therapy
PapersDesign, Synthesis, and Evaluation of Lipopeptide Conjugates of Mercaptoundecahydrododecaborate for Boron
Neutron Capture Therapy
A. Isono, M. Tsuji, Y. Sanada, A. Matsushita, S. Masunaga, T. Hirayama and H. Nagasawa
ChemMedChem 14(8) (2019) 823-832.
Development of proton beam irradiation system for small animals using FFAG accelerator
H. Tanaka, T. Takata, Y. Ishi, T. Uesugi, Y. Kuriyama, T. Watanabe, Y. Sakurai, S. Kawabata, S.-I. Masunaga and
M. Suzuki.
Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors andAssociated Equipment 922 (2019) 230-234.
Depth distributions of RBE-weighted dose and photon-isoeffective dose for boron neutron capture therapy
T. Sato, S.-I. Masunaga, H. Kumada and N. Hamada
Radiation Protection Dosimetry 183(1-2) (2019) 247-250.
Intracellular target delivery of cell-penetrating peptide-conjugated dodecaborate for boron neutron capture therapy(BNCT)
I. Nakase, M. Katayama, Y. Hattori, M. Ishimura, S. Inaura, D. Fujiwara, T. Takatani- Nakase, I. Fujii, S. Futaki
and M. Kirihata
Chemical Communications 55(93) (2019) 13955-13958.
Preparation of pentagamaboronon-0 and its fructose and sorbitol complexes as boron carrier for boron neutron
capture therapy (BNCT) application
E. Meiyanto, R.A. Susidarti, R.Y. Utomo, L. Qodria, R.D. Ramadani, Y. Ohta, Y. Hattori and M. Kirihata
Research in Pharmaceutical Sciences 14(4) (2019) 286.
A design study of application of the CsI self-activation method to the neutron rem-counter techniqueT. Ueki, A. Nohtomi, G. Wakabayashi, J. Fukunaga, T. Kato and S. Ohga
Radiation Measurements 128 (2019) 106181.
Usefulness of combination with both continuous administration of hypoxic cytotoxin and mild temperature
hyperthermia in boron neutron capture therapy in terms of local tumor response and lung metastatic potential
S.I. Masunaga, Y. Sakurai, H. Tanaka, T. Takata, M. Suzuki, Y. Sanada, K. Tano, A. Maruhashi and K. Ono
International Journal of Radiation Biology 95(12) (2019) 1708-1717.

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In Vitro Evaluation System of Pharmacokinetics and Irradiation Effect in Boron Neutron Capture Therapy (BNCT)
Using Three-Dimensional Artificial Human Tumor Tissue Model
S. Ishiyama, Y. Asano, M. Suzuki, A. Mitsuru and H. Shimoda
Journal of Cancer Therapy 10(10) (2019) 835-845.
Radiation Sensitivity of in Vitro Evaluation System of Pharmacokinetics in Boron Neutron Capture Therapy (BNCT)
Using Three-Dimensional Artificial Human Tumor Tissue Model
S. shiyama and M. Suzuki
Journal of Cancer Therapy 10(12) (2019) 1025-1035.
Boron neutron capture therapy (BNCT): a unique role in radiotherapy with a view to entering the accelerator-based
BNCT era
M. Suzuki
International Journal of Clinical Oncology 25(1) (2020) 43-50.
Boron nitride (10BN) a prospective material for treatment of cancer by boron neutron capture therapy (BNCT)
M. Kaur, P. Singh, K. Singh, U.S. Gaharwar, R. Meena, M. Kumar, F. Nakagawa, S. Wu, M. Suzuki, H. Nakamura
and A. Kumar
Materials Letters 259 (2020) 126832.
Poly(vinyl alcohol) boosting therapeutic potential of p-boronophenylalanine in neutron capture therapy bymodulating metabolism
T. Nomoto, Y. Inoue, Y. Yao, M. Suzuki, K. Kanamori, H. Takemoto, M. Matsui, K. Tomoda and N. Nishiyama
Science Advances 6(4) (2020) eaaz1722.
Design and construction of an accelerator-based boron neutron capture therapy (AB-BNCT) facility with multiple
treatment rooms at the Southern Tohoku BNCT Research Center
T. Kato, K. Hirose, H. Tanaka, T. Mitsumoto, T. Motoyanagi, K. Arai, T. Harada, A. Takeuchi, R. Kato, S. Yajima
and Y. Takai
Applied Radiation and Isotopes 156 (2020) 108961.
Enhanced MRI-Guided Gadolinium (III) Neutron Capture Therapy by Polymeric Nanocarriers Promoting Tumor
Accumulation and Intracellular Delivery
C. Qin, X. Hou, T. Khan, N. Nitta, M. Yanagawa, Y. Sakurai, M. Suzuki, S.䇲I. Masunaga, H. Tanaka, Y. Sakurai,
H. Takahashi, I. Aoki, H. Yanagie and H. Cabral
ChemNanoMat 6 (3) (2020) 412-419.
Growth and scintillation properties of a new red-emitting scintillator Rb2HfI6 for the fiber-reading radiation monitor
S. Kodama, S. Kurosawa, Y. Morishita, H. Usami, T. Torii, M. Hayashi, M. Sasano, T. Azuma, H. Tanaka, V.
Kochurikhin, J. Pejchal, R. Kra , M. Yoshino, A. Yamaji, S. Toyoda, H. Sato, Y. Ohashi , Y. Yokota, K. Kamada,
M. Nikl and A. Yoshikawa
IEEE TRANSACTIONS ON NUCLEAR SCIENCE 2020.
Carrier proteins-based boron delivery to tumor
S. Kikuchi, S. Sato and H. Nakamura
Applied Radiation and Isotopes 157 (2020) 109011.
Evaluation of PHITS for microdosimetry in BNCT to support radiobiological research
N. Hu, H. Tanaka, T. Takata, S. Endo, S. Masunaga, M. Suzuki and Y. Sakurai
Applied Radiation and Isotopes 161 (2020) 109148.
Fiber-read radiation monitoring system using an optical fiber and red-emitting scintillator for ultra-high-dose
conditions
S. Kodama, S. Kurosawa, M. Ohno, Y. Morishita, H. Usami, M. Hayashi, M. Sasano, T. Azuma, H. Tanaka, V.
Kochurikhin, A. Yamaji, M. Yoshino, S. Toyoda, H. Sato, Y. Ohashi, K. Kamada, Y. Yokota and A. Yoshikawa
Applied Physics Express 13(4) (2020) 047002.
Microdosimetric quantities of an accelerator-based neutron source used for boron neutron capture therapy measured
using a gas filled proportional counter
N. Hu, H. Tanaka, T. Takata, K. Okazaki, R. Uchida and Y. Sakurai
Jounal of radiation research 61(2) (2020) 214-220.

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Clinical results: patients with head and neck squamous cell carcinoma who have no other treatment options.
-Japanese experiencesI. Kato
Neutron Capture Therapy - Principles and Applications (2nd edition): Wolfgang Sauerwein, Andrea Wittig,
Ray Moss, Yoshinobu Nakagawa, Koji Ono Editors (2020) in press.
Proceedings
Synthesis and Biological Evaluation of S-Octylsulfoniododecaborate Containing L-Amino Acids for Boron Neutron
Capture Therapy
Y. Hattori, M. Ishimura, Y. Ohta, H. Takenaka, K. Matsumoto, K. Uehara, T. Asano and M. Kirihata
Peptide Science 2019 Tokyo, Japan (Oct.23-25, 2019).
᪂つ䝩䜴⣲⸆๣㛤Ⓨ䛻ྥ䛡䛯◊✲㛤Ⓨ/
Preclinical study for development of new drug for NCT
M. Suzuki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 1. (in Japanese)
BNCT 㐺ᛂᣑ኱䛻ྥ䛡䛯᥈⣴ⓗ⮫ᗋ◊✲/Clinical research on explorations into new application of BNCT
M. Suzuki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 2. (in Japanese)⤒㊰㜼ᐖ๣䛿ᨺᑕ⥺↷ᑕ䛸ᢠ PD1 ᢠయ㜼ᐖ๣䛾ే⏝ຠᯝ䜢 NK ⣽⬊䞉CD8+T ⣽⬊䜢௓䛧䛶ቑᙉ䛩䜛/
Better early NK and CD8+T cell-dependent tumor control by adding IDO pathway inhibitor to hypofractionatedradiotherapy plus Anti-PD1 checkpoint blockade
T. Watanabe, G. Niedermann and M.Suzuki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 3-5. (in Japanese)
BNCT 䛻㛵䛩䜛⥲ྜⓗ⥺㔞ホ౯䝅䝇䝔䝮䛾ᵓ⠏/
Establishment of integrated system for dose estimation in BNCTY. Sakurai, A. Uritani, M. Ishikawa, A. Nohtomi, S. Endo, K. Tanaka, K. Shinsho, M. Oita, S. Hayashi, H. Tanaka,
S. Kurosawa, T. Tanimori, S. Nakamura, T. Takata, H. Yasuda, S. Uno, H. Michiue and I. Murata
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 6-10. (in Japanese)䝩䜴⣲୰ᛶᏊᤕᤊ⒪ἲ⏝᪂つ䝩䜴⣲⸆๣㏦㐩䝒䞊䝹䛸䛧䛶䛾஧㔜≉␗ᛶᢠయ䛾ᢠཎㄆ㆑⬟/Recognition of double antigen by using a bispecific antibody for boron delivery in boron neutron capture therapy
T. Kanai, T. Tachibana, T. Nakanishi and T. Nagasaki
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 18. (in Japanese)Hif-1α 㑇ఏᏊḞᦆ䛜 BNCT 䛾ẅ⣽⬊ຠᯝ䜢ቑᙉ䛩䜛/
Disruption of Hif-1α enhances the sensitivity to BNCT in murine squamous cell carcinoma
Y. Sanada, T. Takata, Y. Sakurai, H. Tanaka, K. Tano and S. Masunaga
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 38. (in Japanese)
Reviews୰ᛶᏊᤕᤊ⒪ἲ䛾䛯䜑䛾䝩䜴⣲⸆๣◊✲㛤Ⓨ䛾㐍ᒎ : 䝩䜴⣲⸆๣䛜௒ᚋ䛾㐺ᛂ⑌ᝈᣑ኱䛾㘽䜢ᥱ䜛! (ᙺ䛻❧䛴ᨺᑕ⥺ : ་⒪䜈䛾฼⏝)/
Recent Advances in the Development of Boron Agents for Neutron Capture Therapy୰ᮧ ᾈஅ䜰䝖䝰䝇 : ᪥ᮏཎᏊຊᏛ఍ㄅ/Ατομοσ : journal of the Atomic Energy Society of Japan 62(1) (2020) 18-22. (in Japanese)⓶⭵ᝏᛶ⭘⒆䛻ᑐ䛩䜛䝩䜴⣲୰ᛶᏊᤕᤊ⒪ἲ䠄BNCT䠅䛾⌧≧ᖹሯ⣧୍, ⚄㇂ఙᙪ, Ἑ⏣⿱஧㑻, ➲ᒸಇ㍜, ᱓ཎ༓ᬗ, ⏣୰஢Skin Cancer 34(2) (2019) 116-120. (in Japanese)‑316‑䛆α ⥺἞⒪䛸 DDS䛇4.䝩䜴⣲୰ᛶᏊᤕᤊ⒪ἲ䠖䛜䜣⣽⬊ෆ䛷䃐⥺䜢Ⓨ⏕䛥䛫䜛ḟୡ௦ᨺᑕ⥺἞⒪୰ᮧᾈஅDDS Ꮫ఍ㄅ 35(2) (2020) 129-136. (in Japanese)䛆α ⥺἞⒪䛸 DDS䛇5.ᝏᛶ㌾㒊⭘⒆䜈䛾᪂䛯䛺἞⒪䜸䝥䝅䝵䞁䛸䛧䛶䛾୰ᛶᏊᤕᤊ⒪ἲ䛾⌧≧䛸ྍ⬟ᛶᏳ⸨ ᚭ, ᕷᕝ ⚽႐, ⸨ᮏ ༟ஓ, 㕥ᮌ ᐇ
DDS Ꮫ఍ㄅ 35(2) (2020) 137-145. (in Japanese)ຍ㏿ჾ୰ᛶᏊ※䜢⏝䛔䛯୰ᛶᏊᤕᤊ⒪ἲ䛾⌧≧䛸௒ᚋ䛾ᒎᮃ୰ᮧᾈஅ
BIO Clinica 34 (2019) 431-434. (in Japanese)᭷ᮃ䛺ᨺᑕ⥺἞⒪䛻䛴䛔䛶బ䚻ᮌⰋᖹ, ฟỈ♸௓, ྜྷᮧு୍, ຍ⸨㐓㑻㻌᪥ᮏཱྀ⭍⭘⒆Ꮫ఍ㄅ 32(4) (2019). (in Japanese)

8. Neutron Radiography and Radiation Application
Papers
Effects of p53 Status of Tumor Cells and Combined Treatment With Mild Hyperthermia, Wortmannin or Caffeine
on Recovery From Radiation-Induced Damage
S.-I. Masunaga, K. Tano, Y. Sanada, M. Suzuki, A. Takahashi, K. Ohnishi and K. Ono
World Journal of Oncology 10(3) (2019) 132-141.
୰ᛶᏊ䜲䝯䞊䝆䞁䜾䜢⏝䛔䛯㧗ᙉᗘ䝁䞁䜽䝸䞊䝖ෆ㒊䛾⬺Ỉ䛻㛵䛩䜛◊✲ᑠᒣᣅ䠈すᑿᝆᖹ䠈ఀ⸨኱௓䠈වᯇᏛ䝁䞁䜽䝸䞊䝖ᕤᏛㄽᩥ㞟 41 (2019) 1013-1018. (in Japanese)
An experimental setup for creating and imaging 4He2* excimer cluster tracers in superfluid helium-4 via neutron3
He absorption reaction
V. Sonnenschein, Y. Tsuji, S. Kokuryu, W. Kubo, S. Suzuki, H. Tomita, Y. Kiyanagi, T. Iguchi, T. Matsushita, N.
Wada, M. Kitaguchi, H. Shimizu, K. Hirota, T. Shinohara, K. Hiroi, H. Hayashida, W. Guo, D. Ito and Y. Saito
Review of Scientific Instruments 91(3) (2020) 033318.
Proceedings
Development of multiphase flow imaging technique using neutrons and x-ray
D. Ito, K. Ito and Y. Saito
Proceedings of the 10th International Conference on Multiphase Flow Rio de Janeiro, Brazil (May19-24, 2019).
Velocity vector measurement of LBE flows by using neutron imaging
Y. Saito and D. Ito
Proceedings of the 10th International Conference on Multiphase Flow Rio de Janeiro, Brazil (May19-24, 2019).
Design and Construction of an Imaging beamline at the Nagoya University Neutron Source
K. Hirota, S. Awano, T. Fujiie, S. Fukumura, M. Hishida, G. Ichikawa, S. Imajo, I. Itoh, Y. Iwashita, M. Kitaguchi,
Y Kiyanagi, Y. Kuriyama, K. Morikawa, Y. Niinomi, H. M. Shimizu, K. Tsuchida, Y. Tsuchikwa, Y. Tsurita, A.
Uritani, K. Watanabe, Y. Yamagata, N. Yamamoto, A. Yamazaki, S. Yoshihashi and T. Yoshioka
8th International Meeting of Union for Compact Accelerator-Driven Neutron Sources䠄UCANS8䠅Paris, France(July 8-10, 2019).
Improvement of high-speed neutron imaging for visualization of reflooding phenomena
D. Ito, K.Ito and Y. Saito
Proceedings of Specialists Workshop on Advanced Instrumentation and Measurement Techniques for Experiments
related to Nuclear Reactor Thermal Hydraulics and Severe Accidents Livorno, Italy (Oct.22-25, 2019).
Effects of water distribution on the electrical characteristics of polymer electrolyte fuel cell
H. Murakawa, S. Sakihara, A. Shirakawa, K. Sugimoto, H. Asano, D. Ito and Y. Saito
Proceedings of International Conference on Power Engineering-2019 Kunming, China (Oct.21-25, 2019) 1081-1084.

‑317‑

Evaluationof Meltwter Behavior During the Defrosting Process by Using X-ray radiography
T. Shiokawa, R. Matsumoto, Y. Nishiura, Y. Saito and D. Ito
Proceedings of the 2019 Energy and Refrigerating Air-Conditioning Conference Taipei, TAIWAN ERAC2019(Oct.26-27, 2019) IS003.
X-Ray Radiography and Numerical Simulation of Gas Bubble Behavior in Centrifugal Pump
R. Xiong, K. Ito, D. Ito, Y. Saito, H. Ushifusa, M. Shinozaki, Y. Asai and M. Sato
Proceedings of the 11th International Symposium on Measurement Techniques for Multiphase Flow
Zhenjiang, Jiangsu, China (Nov.3-17, 2019).
Quantitative Measurement of Reflooding Process by Using Neutron Radiography
H. Umekawa, K. Saito, H. Fujiwara, H. Sakai, T. Ami, Y. Saito and D. Ito
Proceedings of the 11th International Symposium on Measurement Techniques for Multiphase Flow
Zhenjiang, Jiangsu, China (Nov.3-17, 2019).

9. TRU and Nuclear Chemistry
PapersMeasurements of thermal-neutron capture cross-section and resonance integral of neptunium-237
S. Nakamura, F. Kitatani, A. Kimura, A. Uehara and T. Fujii
Journal of Nuclear Science and Technology 56(6) (2019) 493-502.
Enhanced Thermoelectric Properties of Ga and Ce Double-Filled p-Type Skutterudites
J. Kim, Y. Ohishi, H. Muta and K. Kurosaki
MATERIALS TRANSACTIONS 60(6) (2019) 1078-1082.
Structural Approach to Understanding the Solubility of Metal Hydroxides
T. Kobayashi, S. Nakajima, R. Motokawa, D. Matsumura, T. Saito and T. Sasaki
Langmuir 35(24) (2019) 7995-8006.
Iodine-rich mixed composition perovskites optimised for tin(iv) oxide transport layers: the influence of halide ion
ratio, annealing time, and ambient air aging on solar cell performance
M. Ozaki, Y. Ishikura, M.A. Truong, J. Liu, I. Okada, T. Tanabe, S. Sekimoto, T. Ohtsuki, Y. Murata, R. Murdey
and A. Wakamiya
Journal of Materials Chemistry A 7(28) (2019) 16947-16953.
Leaching behavior of gamma-emitting fission products, calcium, and uranium from simulated MCCI debris in water
T. Sasaki, S. Sakamoto, D. Akiyama, A. Kirishima, T. Kobayashi and N. Sato
Journal of Nuclear Science and Technology 56(12) (2019) 1092-1102.
Spin-triplet superconductivity in the paramagnetic UCoGe under pressure studied by 59Co NMR
M. Manago, S. Kitagawa, K. Ishida, K. Deguchi, N. K. Sato and T. Yamamura
Physical Review B 100(3) (2019) 035203.
Effects of the nuclear structure of fission fragments on the high-energy prompt fission γ-ray spectrum in U235(nth,f)H. Makii, K. Nishio, K. Hirose, R. Orlandi, R. Léguillon, T. Ogawa, T. Soldner, U. Köster, A. Pollitt, F.-J. Hambsch,
I. Tsekhanovich, M. Aïche, S. Czajkowski, L. Mathieu, C. M. Petrache Astier A.,Guo S., T. Ohtsuki, S. Sekimoto,K. Takamiya, R.JW_Frost and T. Kawano.
Physical Review C 100(4) (2019) 44610.
Neutron activation analysis of carbonate reference materials: coral (JCp-1) and giant clam (JCt-1)
S. Sekimoto, Y. Homura, V. D. Ho, M. Inagaki, N. Shirai and T. Ohtsuki
Journal of Radioanalytical and Nuclear Chemistry 322 (2019) 1579-1583.
Superconductivity at the Pressure-Induced Ferromagnetic Critical Region in UCoGe
M. Manago, S. Kitagawa, K. Ishida, K. Deguchi, N. K. Sato and T. Yamamura
Journal of the Physical Society of Japan 88(11) (2019) 113704.
Thermodynamic interpretation of uranium(IV/VI) solubility in the presence of α-isosaccharinic acid
T. Kobayashi, T. Sasaki and A. Kitamura
The Journal of Chemical Thermodynamics 138 (2019) 151-158.

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Direct observation of vanadium ion permeation behavior through Nafion 117 using 48V radiotracer for
all-vanadium redox flow battery
K. Shirasaki and T. Yamamura
Journal of Membrane Science 592 (2019) 117367.
Production of 47Sc, 67Cu, 68Ga, 105Rh, 177Lu, and 188Re using electron linear accelerator
M. Inagaki, S. Sekimoto, W. Tanaka, T. Tadokoro, Y. Ueno, Y. Kani and T. Ohtsuki
Journal of Radioanalytical and Nuclear Chemistry 3 (2019) 1703-1709.
Dispersal Rate of Radon-219 from Aqueous Radium-223 Solution Containing Sodium Chloride/Citrate
K. Nagata, K. Shirasaki, A. Toyoshima, K. Ooe, T. Yamamura, A. Shinohara and T. Yoshimura
Radiation Safety Management 19 (2020) 1-9.
Proceedings໬Ꮫ஺᥮ἲ䛻䜘䜛䝰䝸䝤䝕䞁ྠ఩య⃰⦰/
Isotope separation of Molybdenum by chemical exchange method
K. Tanoshiro, C.Kato, S. Fukutani, S. Sekimoto, T. Otsuki, T. Ohno, S. Umehara and T. Fujii
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 15. (in Japanese)
MA/REE ศ㞳⏝ᢳฟ๣䜢⏝䛔䛯ᕼᅵ㢮ඖ⣲䛾ᢳฟᶵᵓ䛻㛵䛩䜛◊✲/Research on extraction mechanism of rare earth elements using extractants for MA/REE separation
Y. Yoneda, T. Kawakami, S. Ogawa, T. Matsumura, H. Suzuki, S. Fukutani, C. Kato and T. Fujii
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 17. (in Japanese)䝜䞊䝧䝸䜴䝮◊✲䛻ྥ䛡䛯䠎᪘ඖ⣲䛾Ỉ㓟໬≀䛚䜘䜃◲㓟ỿẊᐇ㦂/Hydroxide and sulfate precipitation experiment of Group 2 elements toward the chemical study of nobelium
S. Hayami, E. Watanabe, H. Ninomiya, K. Tonai, Y. Kasamatsu and A. Shinohara.
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 22. (in Japanese)౑⏝῭䜏⇞ᩱ෌ฎ⌮ᕤ⛬䛻䛚䛡䜛䝰䝸䝤䝕䞁䛾㓟໬㑏ඖᣲື/
Redox behavior of molybdenum in spent fuel reprocessing process
S. Shinya, S. Yatsugi, H. Sugihara, A. Uehara, C. Kato and T. Fujii
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 39. (in Japanese)᪂つᢳฟ๣䜢⏝䛔䛯◪㓟⁐ᾮ䛛䜙䛾䝉䝺䞁䛾⁐፹ᢳฟ≉ᛶ/
Solvent extraction of selenium in nitric acid solutions using novel extractants
T. Kawakami, Y. Yoneda, S. Ogawa, T. Matsumura, Y. Tsubata, K. Morita, S. Fukutani, A. Uehara, C. Kato andT. Fujii
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 45. (in Japanese)◪㓟⁐ᾮ䛻⁐Ꮡ䛩䜛䝞䝘䝆䜴䝮䛾ศග㟁Ẽ໬Ꮫศᯒ/Spectroelectro-chemical study of vanadium in nitric acid solution
S. Yatsugi, A. Uehara, S. Sato, H. Sugihara, C. Kato and T. Fujii
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 47. (in Japanese)ᶍᨃ⇞ᩱ䝕䝤䝸䛾⁐ฟ䛻㛵䛩䜛ᐇ㦂ⓗ◊✲ /Experimental study on leaching behavior from simulated fuel debris
R. Tonna, Y. Kodama, T. Kobayashi, T. Sasaki, N. Sato, A. Kirishima, D. Akiyama, S. Sekimoto and R. Okumura
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 49. (in Japanese)໬Ꮫ஺᥮ἲ䛻䛚䛡䜛ྠ఩యศู◊✲/Study of isotope separation via chemical exchange reaction
R. Hazama, T. Yoshimoto, Y. Sakuma, T. Fujii, S. Fukutani and Y. Shibahara
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 51. (in Japanese)

10. Health Physics and Waste Management
PapersDEVELOPMENT OF A PELTIER TYPE CLOUD CHAMBER WITH WIDE VIEW FIELD
T. Toda, M.M. Hasan, Y. Igarashi, E.W. Katengeza and T. Iimoto
Radiation Protection Dosimetry 184(3-4) (2019) 539-542.

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䝁䝻䜲䝗䛾Ꮡᅾ䜢⪃៖䛧䛯 Cs 䛾᳃ᯘᅵተ୰⛣ື䝯䜹䝙䝈䝮䛻㛵䛩䜛◊✲ᓥ⏣ ὒᏊ, ୗᕝ ㄹ, ⡿⏣ ⛱, ụୖ 㯞⾰Ꮚ, ⚟㇂ ဴ, 㣁⏣ ᑦဢ, Ⳣཎ ኱㍜ᅵᮌᏛ఍ㄽᩥ㞟 G䠄⎔ቃ䠅 75 (2019) 117-125. (in Japanese)
Iron oxide nanoparticle core-shell magnetic microspheres: Applications toward targeted drug delivery
S. Ayyanaar, M.P. Kesavan, C. Balachandran, S. Rasala, P. Rameshkumar, S. Aoki, J. Rajesh, T.J. Webster and G.
Rajagopal
Nanomedicine: Nanotechnology, Biology and Medicine 24 (2020) 102134.
Proceedings
Current Status of KURAMA-II
M. Tanigaki
Proceedings of 17th Biennial International Conference on Accelerator and Large Experimental Physics Control
Systems New York, USA (Oct.5-11, 2019) 1-3.
Nuclear Waste lnventory Calculations from Fuel Cycle with Fast Reactors by a Reactor Physics Code System CBZ
Y. Kobayashi and G. Chiba
Proceedings of Reactor Physics Asia Conference 2019 (RPHA2019) Osaka, Japan (Dec.2-3, 2019) 123-126.
ሜᕷ䛷ほ 䛧䛯኱Ẽ䜶䜰䝻䝌䝹⢏ᚄูඖ⣲ᡂศ䛾㛗ᮇほ ⤖ᯝ/Long term observation of element concentration in the atmospheric aerosols at Sakai, Osaka,1995-2017
N. Ito, A. Mizohata, Y. Iimura and R. Okumura
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 16. (in Japanese)䝠䝇䝖䞁䝞䝸䜰䞁䝖 H2A.B 䜢ྵ䜐䝚䜽䝺䜸䝋䞊䝮䛾⮬Ⓨⓗ䛺䝠䝇䝖䞁஺᥮ᶵᵓゎᯒ/
Spontaneous histone exchange activity of histone variant H2A.B nucleosome
R. Hirano, Y. Arimura, T. Kujirai, R. Inoue, A. Okuda, K. morishima, M. Sugiyama and H. Kurumizaka
Proceedings of the 54th KURNS Scientific Meeting Kumatori, Japan (Feb.5-6, 2020) 31. (in Japanese)
Prediction of Municipal Solid Waste Composition and Estimation of Impact on Incineration Process in Depopulation
and Aging Society
S. Hayasaki, K. Oshita, K. Kawai and M. Takaoka
The 6th 3R International Scientific Conference on Material Cycles and Waste Management Tsukuba, JAPAN(Mar.16-18).
Review
Activities and Development for NS&T HRD Focusing on Secondary School Levels in Asia Pacific Region _Case ofJapan
T. Iimoto, T. Kakefu, R. Takaki, T. Toda, I. Takahashi, G. Wakabayashi, H. Iizuka, K. Makabe and T. Koashi
Journal of Radiation Emergency Medicine 8(1) (2019) 33-38.
Application of a Hand-made Air GM Counter as a Radiation Education Training Material for Secondary School
Education
E. W. Katengeza, R. A. C. N. Ranasinghe, S. Ozaki and T. Iimoto
Japanese Journal of Health Physics 54(4) (2020) 206-211.
ᅜ㝿つไ≀㈨䠄ᑡ㔞᰾⇞ᩱ≀㉁䠅䛻ಀ䜛ᩍ⫱䛾䛒䜚᪉/Concept of Internal Education Regarding the Use of International Controlled Material for Small Amount of Nuclear
MaterialsᏳ⏣ ᖾྖ, 㧗ᶫ ㈼⮧, 㣤ᮏ Ṋᚿ, ᮌᮧ ᆂᚿ, ✄ᇉ ᫀ௦, ᒣす ᘯᇛ /K. Yasuda, M. Takahashi, T. Iimoto, K. Kimura, M. Inagaki and H. Yamanishi
RADIOISOTOPES 69(2) (2020) 55-65.
Development of radiation literacy among secondary school students in SRI LANKA
N. Ranasinghe,㻌 U. Perera, P. Mahakumara, N. Rathnaweera, P. Rathnayake, T.Toda and T. Iimoto
Journal of Environment and Safety 10(2) (2019) 37-40.

11. Accelerator Physics
PapersAC Losses in HTS Coils of Superferric Dipole and Combined-Function Magnets
Y. Sogabe, M. Yasunaga, Y. Fuwa, Y. Kuriyama, T. Uesugi, Y. Ishi and N. Amemiya
IEEE Transactions on Applied Superconductivity 29(5) (2019) 8629310.

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Proceedings
Beam Optics Study on FFA-MERIT Ring
H. Okita, Y. Ishi, Y. Kuriyama, Y. Mori, Y. Ono, A. Taniguchi, T. Uesugi, N. Ikeda, Y. Yonemura, M. Kinsho, K.
Okabe, M. Yoshimoto, Y. Miyake, M. Muto and A. Sato
10th International Particle Accelerator Conference (IPAC2019) Melbourne, Australia (May19-24, 2019).
Remodeling of 150 MeV FFAG Main Ring at KURNS to Pion Production Ring
K. Suga, Y. Fuwa, Y. Ishi, Y. Kuriyama, Y. Mori, H. Okita and T. Uesugi
10th International Particle Accelerator Conference (IPAC2019) Melbourne, Australia (May19-24, 2019).
Longitudinal Tomography in a Scaling FFA
D.J. Kelliher, C. Brown, J.-B. Lagrange, S. Machida, C.R. Prior, C.T. Rogers, Y. Ishi, Y. Kuriyama, H. Okita,
T. Uesugi and S.L. Sheehy
10th International Particle Accelerator Conference (IPAC2019) Melbourne, Australia (May19-24, 2019).
Study of Beam Injection Efficiency in the Fixed Field Alternating Gradient Synchrotron at KURNS
T. Uesugi, Y. Fuwa, Y. Ishi, Y. Kuriyama, Y. Mori, H. Okita and K. Suga
10th International Particle Accelerator Conference (IPAC2019) Melbourne, Australia (May19-24, 2019).
Updates on the Inspection System for SRF Cavities
Y. Iwashita, H. Tongu, H. Hayano and Y. Kuriyama
The 19th International Conference on RF Superconductivity (SRF2019) Dresden, Germany (Jun.30-July5, 2019).
Proposal of a 1-ampere-class deuteron single-cell linac for nuclear transmutation
H. Okuno, H. Sakurai, Y. Mori, R. Fujita and M. Kawashima
Proceedings of the Japan Academy, Series B (July, 2019) 430-439.
Recent Experimental Results of the Accelerator Drive System with a Sub-Critical Nuclear Reactor (ADS) Program
Y. Ishi, Y. Fuwa, Y. Kuriyama, Y. Mori, H. Okita, K. Suga and T. Uesugi
International Conference on Cyclotrons and their Applications䠄CYC2019䠅CapeTown, South Africa (Sept.22-27,
2019).

12. Others
Papers」㞧䛺 3 ḟඖἼືሙ䛾 P,SV ཬ䜃 SH Ἴ䜈䛾ᆅ⾲㠃ᆅ㟈ື䜢⏝䛔䛯ศ㞳䠄ᩘ್ᐇ㦂䛻ᇶ䛵䛟᫬㛫䠉✵㛫㡿ᇦ䛻䛚䛡䜛ᡭἲ䛾ホ౯䠅/DECOMPOSITION OF SURFACE SEISMOGRAMS IN THE COMPLEX FULL-WAVEFIELD INTO P-, SVAND SH-WAVES
ୖᯘᏹᩄ/Hirotoshi UEBAYASHI᪥ᮏᘓ⠏Ꮫ఍ᵓ㐀⣔ㄽᩥ㞟/Journal of Structural and Construction Engineering (Transactions of AIJ) 18(5) 513 (2019) 521. (in Japanese)
Determination of the electric field gradient tensor of Fe3+ in the M1 site of aegirine by single crystal Mössbauer
spectroscopy
K. Shinoda and Y. Kobayashi
Journal of Mineralogical and Petrological Sciences 114(3) (2019) 130-141.
CubeSat bus interface with Complex Programmable Logic Device
T. Tumenjargal, S. Kim, H. Masui and M. Cho
Acta Astronautica 160 (2019) 331-342.
Development of Near-Infrared Fluorescent Probes with Large Stokes Shifts for Non-Invasive Imaging of Tumor
Hypoxia
H. Nagasawa, K. Okuda, B. G. M. Youssif, R. Sakai, T. Ueno, T. Sakai, T. Kadonosono, Y. Okabe, O. I. A. R.
Salem, A. M. Hayallah, M. A. Hussein and S. Kizaka-Kondoh
HETEROCYCLES 101(2) (2019) 559.

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PD-L1 and PD-L2 expression in the tumor microenvironment including peritumoral tissue in primary central nervous
system lymphoma
M. Furuse, H. Kuwabara, N. Ikeda, Y. Hattori, T. Ichikawa, N. Kagawa, K. Kikuta, S. Tamai, M. Nakada, T.
Wakabayashi, M. Wanibuchi, T. Kuroiwa, Y. Hirose and S.-I. Miyatake
BMC Cancer 20(1) (2020) 277.
The effect of body waves on phase-velocity determined by the spatial autocorrelation (SPAC) method, evaluatedusing full-wave modelling
H. Uebayashi, I. Cho, M. Ohori, K. Yoshida and H. Arai
Exploration Geophysics 1 (2020) 11.
䝁䝠䞊䝺䞁䝖ඹ㬆ᚋ᪉ᅇᢡᨺᑕ䛻䜘䜛‽༢Ⰽ䝔䝷䝦䝹䝒ග※䛾◊✲Ύ ⣖ᘯ䠈㧗ᶫಇᬕ᪥ᮏ㉥እ⥺Ꮫ఍ㄅ 29(2) (2020) 49-56. (in Japanese)
Design, Synthesis, and Conformation䇵Activity Study of Unnatural Bridged Bicyclic Depsipeptides as Highly Potent
Hypoxia Inducible Factor-1 Inhibitors and Antitumor Agents
K. Koike, M. Nagano, M. Ebihara, T. Hirayama, M. Tsuji, H. Suga and H. Nagasawa
Journal of Medicinal Chemistry 63(8) (2020) 4022-4046.
High-count-rate 3He position-sensitive detector system: NEUNET-HCR
S. Sato, T. Seya, H. Oshita, H. Kato, N. Hikida, K, Ishizawa, A. Yamaguchi and M. Matsuura
EPJ Web of Conferences 231 (2020) 05004.
Proceedings
Research of coherent edge radiation generated by electron beams oscillating free-electron lasers
N. Sei, H. Ogawa, T. Tanaka, Y. Hayakawa, T. Sakai, Y. Sumitomo, Y. Takahashi, K. Hayakawa, K. Nogami,
H. Zen and H. Ohgaki
Journal of Physics: Conference Series Conference Melbourne, Australia (May19-24, 2019) 12039.
The change in characteristics of soil and Cs elution by heat treatment
M. Ikegami, K. Kuroki, S. Fukutani, Y. Shimada and M. Yoneda
5th International Conference on Environmental Radioactivity ENVIRA 2019 Czech (Sept.8-13, 2019) 25-26.
Study of gas-gain saturation and cross-talk effect by low energy proton with a prototype chamber for the COMET
CDC
H. Yoshida, M. Aoki, M. Dobouchet, M. Moritsu, A. Sato, Y, Ishi, Y. Kuriyama, T. Uesugi and Y. Mori
J-PARC Symposium 2019 Tsukuba, Japan (Sept.23-26, 2019).
Books䛜䜣⏕≀Ꮫ䜲䝷䝇䝖䝺䜲䝔䝑䝗㻌 ➨ 2 ∧㏆⸨ ኟᏊ, ᖹ⏣ ⱥ࿘, ῰㇂ ṇྐ, ‫‮‬ὸ ಖோ➨ 9 ❶ 6. ⬻⭘⒆⨺ᅵ♫ (2019). (in Japanese)
Reviewᅜෆእ䛾ཎᏊຊᩍ⫱஦᝟(2)ி㒔኱ᏛཎᏊ᰾ᕤᏛᑓᨷ䞉ཎᏊ᰾ᕤᏛ䝁䞊䝇㧗ᮌ㑳஧, ୰ᓥ೺᪥ᮏཎᏊຊᏛ఍ㄅ䠄䜰䝖䝰䝇䠅61 (2019) 143-145. (in Japanese)ி㒔኱Ꮫ䛂ཎᏊ⅔ᐇ㦂ᡤ䛃䛛䜙䛂」ྜཎᏊຊ⛉Ꮫ◊✲ᡤ䛃䜈/
From Research Reactor Institute to Institute for Integrated Radiation and Nuclear Science, Kyoto Universityᕝ➃♸ྖ/Yuji Kawabataಖ೺≀⌮/Japanese Journal of Health Physics 53(4) (2019) 205-206. (in Japanese)‑322‑

KURNS Progress Report 2019
Issued in $XJXVW 2020
Issued by the Institute for Integrated Radiation and Nuclear Science,
Kyoto University
Kumatori-cho, Sennan-gun, Osaka 590-0494 Japan
Tel. +81-72-451-2300
Fax. +81-72-451-2600

In case that corrections are made, an errata will be provided
in the following webpage:https://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep2019/ProgRep2019.html

Publication TeamIINUMA, Yuto
INOUE, Rintaro (Subchief)
KINASHI, Yuko
KITAMURA, Yasunori
MORI, Kazuhiro (Chief)
NAKAYAMA, Chiyoko
SAKURAI, Yoshinori (Subchief)
SANO, Hiroaki
TAKATA, Takushi
TOMINAGA, Yuta
TSURUTA, Yachiyo
YOKOTA, Kaori‑323‑