ISSN 2189-7093
PRINT ISSN 0919-1038

KURRI
Progress Report

The Research Reactor Institute, Kyoto University

KURRI Progress Report
APRIL 2014 – MARCH 2015

Published by
The Research Reactor Institute, Kyoto University,
Kumatori-cho, Sennan-gun, Osaka 590-0494, Japan

Preface
It is a great pleasure for us to publish the KURRI Progress Report 2014. This report contains all of the accomplishmentsof research and related activities at the Research Reactor Institute, Kyoto University (KURRI) during the fiscal year
2014 from April 2014 to March 2015
The institute was established in 1963 for the joint use program among Japanese universities to promote experimental
research and education in the fields of nuclear energy and radiation application. The main facility, called the Kyoto
University research Reactor (KUR), has been widely used for various experiments since its first criticality in 1964. It
has been successfully operated, and has served as one of the most useful inter-university research reactors in our country.
The Kyoto University Critical Assembly (KUCA), accelerators and other research facilities are also open to researchersand students for their experiments.
In the past fiscal year, KUR was subjected to some facility refurbishments and operated for 360 hours, while KUCA
was not operated. In total, we accepted 3,628 man-day researchers and students for using research facilities and forattending scientific meetings held at KURRI. A large number of research subjects has been enrolled, which covers
various fields of nuclear science and technology, material science, radiation life science and radiation medical science.
It is noted that 30 patients have been treated in the clinical studies of the boron neutron capture therapy (BNCT) using
KUR in this period. The results of these activities are given in this report.
Some special research projects are in progress at KURRI. One is the project on the Accelerator Driven System (ADS)
by using a Fixed Field Alternating Gradient (FFAG) accelerator combined with KUCA. The world’s first ADS
experiment has been successfully conducted on March 2009, and the 150 MeV proton beam is being provided for the
ADS experiment and for the related studies including development of target materials. In another project, the world’s
first clinical trial of the BNCT is being promoted using a proton accelerator, based on the successful clinical studies
using KUR. Such leading research activities as well as educational activities at the institute are highly rated in a recent
external evaluation.
Efficient utilization of nuclear energy and radiation is expected to provide solutions to maintain, sustain and even todevelop human society. However, it is now required to again ensure the safety of nuclear energy for its continued use.
With the joint use of such research resources as reactors and accelerators, our program is thus to strengthen thescientific basis for improved safety and to promote leading research toward efficient utilization of multidisciplinary
nuclear science and technology. Our program also emphasizes the importance of experimental education for fostering
young people in the related fields.
The high standing of the institute in research and related activities relies on the enthusiasm and dedication of all theparticipants. Details of their work and achievements during the year are given in the following pages. I am grateful toall of my colleagues who have taken time to prepare this report, and thank them for their cooperation. Also, I would liketo express my sincere thanks for the continued support from the national and local governments, scientific communities
and residents in the neighborhood of KURRI.

Kumatori, June 14, 2015
Yuji Kawabata
Director, KURRI

CONTENTS
I. ANNUAL SUMMARY OF EXPERIMENTAL RESEARCH ACTIVITIES ................................

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

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Project 1 Analyzing Tumor Microenvironment and Exploiting its Characteristics for Controlling
Malignant Solid Tumors and Distant Metastatic Potential
S. Masunaga (26P1) ························································································
PR1-1
Significance of Fractionated Thalidomide Administration Combined with γ-Ray
Irradiation from the Viewpoint of Local Tumor Response and Lung Metastasis
S. Masunaga et al. (26P1-1) ·········································································
PR1-2
Development of Nuclear-targeting Boron Carriers Based on the Chemistry of Direct
Cell-penetrating Pepducins
A. Isono et al. (26P1-2) ··············································································
PR1-3
Genetic Screening of Upstream Activators of Hypoxia-inducible Factor 1 for the
Devrlopment of Novel Anti-cancer Strategies
H. Harada et al. (26P1-3) ············································································
PR1-4
Quantitative Detection of Metastasized B16BL6 Cells in Lung by Using TaqMan
RT-PCR Assay
T. Nagasaki et al. (26P1-6) ··········································································
PR1-5
Response of Tumor Cells to BNCTS. Imamichi1 et al. (26P1-9) ········································································
PR1-6
Additive effect of Gadolinium to Cell Survival Analysis for Neutron Capture Therapy
K. Nakai et al. (26P1-10) ············································································
Project 2 Direct Observation of the Proton or Protonation in a Protein Molecule by Neutron and High
Resolution X-ray Joint Analysis
Y. Morimoto (26P2) ·······················································································
PR2-1
Degradation Control and Structural Motion of the 20S/26S Proteasome Elucidated by
Genetic Mutation and Atomic Force Microscope
T. Murakami et al. (26P2-1) ·········································································
PR2-2
Development of Improved Techniques for Neutron Biology
T. Chatake et al. (26P2-2) ···········································································
PR2-3
Identification and Characterization of Proteolytic Enzymes Derived from

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NephilaClavata
Y. Hidaka et al. (26P2-3) ············································································
Project 3 Project Research on the New Applicant Development Using the Characteristics of the Particles
from the Neutron Capture Reaction
K. Kinashi (26P3) ·························································································PR3-1
The Effect of Ascorbic Acid on the HPRT Mutation Induction after the Neutron Irradiation
Y. Kinashi et al. (26P3-1) ············································································
PR3-2
Analysis of DNA Double Strand Breaks in the Mammalian Cells Induced by BNCR
S. Takahashi et al. (26P3-2) ·········································································
Project 4 Project Research on Development of Scattering Spctrometers Utilizing Small and Medium
Class Neutron Source
M. Sugiyama (26P4) ······················································································PR4-1
KUR-SANS Observations and Analyses of Surfactants’ Nano-structural Change byCapturing Heavy Metal
K. Hara et al. (26P4-5) ···············································································
Project 5 Behavior of Radioactive Nuclides in Intense Radiation Fields in Accelerator Facilities
Y. Oki (26P5) ······························································································
PR5-1
Radioactivity Size Distribution of Airborne Aerosols Formed in Target Room Estimatedfrom Number Size Distribution
S. Yokoyama et al. (26P5-1) ········································································
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PR5-3

Production of Airborne Nano-Particles by Proton Irradiation in an FFAG Accelerator
Y. Oki et al. (26P5-2) ················································································
Corrosion of Various Metals in Water and Formation of Metal-related Colloidal Particles
under Intense Photon-Raiation Field
K. Bessho et al. (26P5-3) ············································································

Project 6 Irradiation Effects on Nuclear Advanced Materials Irradiated by Particles with High Energy
Q. Xu (26P6) ································································································
PR6-1
PR6-2
PR6-3
PR6-4
PR6-5
PR6-6
PR6-7
PR6-8
PR6-9

PR6-10
PR6-11Compensation Mechanism of DX-like Center in Neutron Transmutation Doped GaN
K. Kuriyama et al. (26P6-1) ··········································································
Neutron Irradiation Effects of Superconducting Magnet Materials at Low Temperature
T. Nakamoto et al. (26P6-2) ··········································································
Study on Fine Structures Formed by High Energy Particle Irradiation
A. Kinomura et al. (26P6-3) ··········································································
Thermoluminescence of Synthesized Calcite
T. Awata et al. (26P6-4) ···············································································
Electron irradiation on W around 500℃ using KURRI-LINAC
M. Akiyoshi et al. (26P6-5) ···········································································The Development of New Positron Beam System Using KUR
Y. Nagai et al. (26P6-6) ···············································································
Radiation Damage in Bulk Amorphous Alloys by Electron Irradiation
F. Hori et al. (26P6-7) ·················································································
Positron Annihilation Study of Fe-Cr Alloys After Neutron Irradiation in KUR
R. Kasada et al. (26P6-10) ············································································
Positron Annihilation Lifetime Measurements of Austenitic Stainless Steels Irradiated in the
SINQ Target Irradiation Program
K. Sato et al. (26P6-12) ···············································································
Effects of High Energy Particle Irradiation on Hydrogen Retention in Refractory Metals
K. Tokunaga et al. (26P6-13) ·········································································
Depenedence of Cellular Structure Formation on Ion Species
N. Nitta et al. (26P6-14)···············································································

Project 8 Development on Neutron Imaging Application
Y. Saito (26P8) ····························································································
PR8-1
Dynamic Observation of Two-Phase Flow Using Neutron Radiography
Y. Saito et al. (26P8-1) ···············································································
PR8-2
Quantitative Measurement of Adsorbed Ethanol Amount in Activated Carbon
Adsorber for Adsorption Heat Pump
H. Asano et al. (26P8-2) ·············································································
PR8-3
Neutron Radiography on Tubular Flow Reactor for Supercritical Hydrothermal
Synthesis of Nanoparticles
T. Tsukada et al. (26P8-3) ···········································································
PR8-4
Neutron Imaging and Optics Development Using Simulation of VCAD Systems
Y. Yamagata et al. (26P8-5) ·········································································
PR8-5
Evaluation of the Moisture Movement in High-Performance Concrete Subjected to Heating
M. Kanematsu et al. (26P8-10) ·····································································
PR8-6
Effect of Gravity on Coolant Distribution in FGHP Heat Spreader
K. Mizuta et al. (26P8-11) ···········································································
PR8-7
Study on Visualization of Organic Materials between Metals for Advance ofIndustrial Products
K. Hirota et al. (26P8-12) ···········································································
PR8-8
Visualization of Flow Inside Fine Scale Wick of Heat Pipe
Y. Tsuji et al. (26P8-13) ··············································································
Project 10 Project Research on the Elucidation of Generating Mechanism of Damaged Protein Induced
by Aging and Irradiation
N. Fujii (26P10) ······················································································

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PR10-2

PR10-3
PR10-4
PR10-5
PR10-6
PR10-7Detection of D-Aspartyl Endopeptidases Activity in Floral Tissues of Broccoli(Brassica oleracea var. Italica)
T. Kinouchi et al. (26P10-1) ··········································································
Damage to Biological Molecules Induced by Ionizing Irradiation and Biological Defense
Mechanisms against Ionizing Radiation I
T. Saito et al. (26P10-2) ···············································································
Analysis of Aspartate Isomerization Using Protein L-Isoaspartyl Methyltransferase (PIMT)
Y. Sadakane et al. (26P10-3) ·········································································
Analysis of Imbalance in Mice Exposed to Environmental Stress
N. Ohgami et al. (26P10-4) ···········································································
Identification of Biologically Uncommon β-aspratyl Residues in Proteins Using MS
N. Fujii et al. (26P10-5) ···············································································Side Chain Conformers of Aspartyl Isomers in Crystallin Mimic Peptide
K. Aki et al. (26P10-6) ················································································
Rapid survey of Asp isomers in disease-related proteins by LC-MS/MS combinedwith Commercial Enzymes
H. Maeda et al. (26P10-7) ············································································

Studies on Actinides and Fission Products Performed at the KURRI Hot Laboratory
T. Fujii (26P11) ··························································································
PR11-1
Apparent Formation Constant of Metal Ions with Humic Substances; Modelling
T. Sasaki et al. (26P11-1) ·············································································
PR11-2Temperature Effect on the Solubility and Solid Phase of Tetravalent Metal Hydroxide
T. Kobayashi et al. (26P11-2) ·······································································
PR11-3
Research on The Behavior of Actinides and FPs in Fuel Debris
N. Sato et al. (26P11-3) ···············································································
PR11-4
Effect on Borosilicate Glass Structure by Neutron Irradiation
T. Nagai et al. (26P11-4) ··············································································
PR11-5
Ligand Exchange of Uranium (IV) Chloro- and Fluoro- Complexes in High Temperature
Molten NaCl-CsCl Eutectic
A. Uehara et al. (26P11-5) ············································································
PR11-6
Evaluation of Parameters Governing Anodic Dissolution of U-Zr Alloy in Molten LiCl-KCl
M. Iizuka et al. (26P11-6) ·············································································
PR11-7
Electrochemistry and Structural Analysis of Cations in Molten Sub-halide Systems:
Fluoride Addition Effect on Voltammograms and UV-vis Spectra of Neodymium Cation in
Molten Chlorides
H. Matsuura et al. (26P11-7) ·········································································
PR11-8Polarization Effect of Chloride Ions on Uranyl Ion in Molten LiCl
N. Ohtori et al. (26P11-8) ·············································································
PR11-9Study of Isotope Separation of Strontium and Calcium via Chemical Exchange Reaction
R. Hazama et al. (26P11-10)··········································································
PR11-10 Experimental and Calculated Optical Properties of Molten Alumnium Chloride Melts
T. Goto et al. (26P11-11) ··············································································
PR11-11 Precipitation Behavior of Trivalent Dysprosium Ion by Reaction with Oxide Ion in
CaCl2–LiCl Molten Salt
H. Sekimoto et al. (26P11-12) ········································································
PR11-12 Elucidation of the Uptake Route of Radionuclides in Deciduous and Coniferous Trees
Using Radio Cesium and Radio Potassium in Annual Tree Rings
T. Ohta et al. (26P11-13) ··············································································
PR11-13 Photon activation analysis of alkali earth elements and arsenic with bremsstrahlungat the KURRI-LINAC
T. Kubota et al. (26P11-14) ···········································································
PR11-14 Study of Applicability of Isotopic Ratio Measurement for Analysis of Radionuclide inEnvironmental Samples
Y. Shibahara et al. (26P11-15) ········································································
PR11-15 Tracing Halogen and Noble Gas Recycling in the Northern Izu Subduction Zone by
Neutron Irradiation and Noble Gas Mass Spectrometry
H. Sumino et al. (26P11-16) ··········································································

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PR11-17

Volcanic and Tectonic History of Philippine Sea Plate (South of Japan) Revealedby 40Ar/39Ar Dating Technique
O. Ishizuka et al. (26P11-17) ·········································································
Ar–Ar Age Determination of Minamitorishima
N. Hirano et al. (26P11-18) ···········································································

Project 12 Project Research on Nuclear Spectroscopy and Condensed Matter Physics Using
Short-Lived Nuclei
Y. Ohkubo (26P12) ······················································································
PR12-1β- Decay of 150Ce to 150Pr
Y. Kojima et al. (26P12-3)············································································
PR12-2
Interaction between He and Elements with A = 140 in Fe
Y. Ohkubo et al. (26P12-4) ··········································································
PR12-3
Atmosphere Dependence of Stability of Local Fields in Al-Doped ZnO
S. Komatsuda et al. (26P12-5)········································································
PR12-4Extranuclear Dynamic Motion of 111Cd(←111Ag) Doped in AgI Nanoparticles
W. Sato et al. (26P12-6) ···············································································
Project 13 Project Research on the Advanced Utilization of Multi-Element Mössbauer Spectroscopy
for the Study of Condensed Matter
M. Seto (26P13) ·························································································
Magnetism of an iron oxypnictide Cr-doped CeFePO
PR13-1T. Okano et al. (26P13-2) ·············································································
PR13-2A study of Formation of Au(III) Surface Complex on Manganese Dioxide by 197Au
Mössbauer Spectroscopy
T. Yokoyama et al. (26P13-3) ·······································································
PR13-3
Mössbauer Spectroscopy of Novel Ferroelectric Materials
S. Nakamura et al. (26P13-5) ·········································································
PR13-4
Mössbauer Spectra of Oriented Thin Sections and Small Grain of Magnetite Single Crystal
T. Kamiryo et al. (26P13-6)···········································································
PR13-5
Electronic States of Negative/Zero Thermal Expansion Materials
I. Yamada et al. (26P13-7) ············································································
Mössbauer Study of Fe-Based Superconductors, Ba1-xKxFe2As2
PR13-6
S. Kitao et al. (26P13-7) ··············································································
Project 14 Translational Research on BNCT for Clinical Application
M. Suzuki (26P14) ······················································································
PR14-1
Boron Neutron Capture Therapy for Radiation-induced Osteosarcoma from the Skull
S. Miyatake et al. (26P14-4) ··········································································
PR14-2Clinical Studies on BNCT for 6 Cases of Head and Neck Cancer
I. Kato et al. (26P14-5) ··············································································
PR14-3
Boron Uptake in Tumour of Local Recurrenced Breast Cancer by 18F-BPA Positron
Emission Tomograpy for Application to Boron Neutron Capture Therapy
H. Yanagie et al. (26P14-8) ···········································································
PR14-4High Boron-Accumulated Liposomes as Efficient Boron Carriers for Neutron
Capture Therapy
H. Nakamura et al. (26P14-16) ·······································································
PR14-5
Boron Carbide Particle as a Boron Compound for BNCT in vivo
S Tada et al. (26P14-18)···············································································
PR14-6
Boron Neutron Capture Therapy Selectively Destroys Human Clear Cell Sarcoma(CCS) Metastasis to Lung in CCS-bearing Animal Model
T. Fujimoto et al. (26P14-19) ·········································································
PR14-7
Nanoparticle-assisted Boron Neutron Capture Therapeutics: Design of Novel
Boron-containing Nanoparticle for ROS Scavenging Ability Improving Therapeutic
Efficiency with Low Adverse Effect
Z. Gaoa et al. (26P14-20) ·············································································
PR14-8
Evaluation of Component in WOW Emulsion as Intra-arterial Boron Delivery Carrier for
Neutron Capture Therapy to Hepatocellular Carcinoma
H. Yanagie et al. (26P14-22)··········································································
iv

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Establishment of QA/QC Using Ionization Chamber and Bonner Sphere in BNCT Field
H. Ueda et al. (26P14-26) ·············································································
Study on the Real-time dose Monitor System Using Prompt Gamma Rays orBoron Neutron Capture Therapy
H. Tanaka et al. (26P14-27) ··········································································
Quality Assurance of Irradiation Field for BNCT Using Twin Imaging Plate System
K. Tanaka et al. (26P14-28) ··········································································Development and Evaluation of 3D Polymer Gel Dosimeter for the Measurement of dose
Distribution in BNCTS. Hayashi et al. (26P14-29) ··········································································

94

I-2. COLLABORATION RESEARCHES ................................................................................................

95

PR14-9PR14-10

PR14-11
PR14-1291
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1. Slow Neutron Physics and Neutron Scattering
CO1-1
CO1-2
CO1-3
CO1-4
CO1-5
CO1-6
CO1-7

Analysis of Heavy Metal Elements in Chinese Medicine and Herbs
E. Furuta et al. (26001) ····················································································
Status Report 2014 for B–3 Beam Port of KUR
K. Mori et al. (26007) ······················································································

Synthesis of Metal Nanoparticles under the Gamma-ray Irradiation Field

96
97

F. Hori et al. (26010) ······················································································· 98
The Role of Human Oxidation Resistance 1 (OXR1) in Cellular Response to Radiation
A. Matsui et al. (26018) ····················································································· 99
Development of an Advanced Optical Fiber Type Neutron Detector
K. Watanabe et al. (26021) ·················································································· 100
Focusing Test of an Ellipsoidal Neutron Mirror with a Metal Substrate
M. Hino et al. (26065) ······················································································· 101
Examination of the Usefulness as the New Boron Compound of KA-BSH for Born Neutron
Capture Therapy
G. Fitamura et al. (26078) ··················································································· 102

2. Nuclear Physics and Nuclear Data
CO2-1

CO2-2
CO2-3
CO2-4

CO2-5

Development of Measurement Method for Epi-Thermal Neutrons Using the 10B(n,)Reaction
T. Matsumoto et al. (26055) ...............................................................................................
Measurement of Gamma Ray and Neutron Spectrum of Curium Isotope (3)Y. Nauchi et al. (26057) ......................................................................................................
Development of Hybrid Ce:LiCAF Scintillator for Nuclear Data Measurement
T. Fujiwara et al. (26058) ...................................................................................................
Investigation of Variable Neutron Field for Accurate Determination of Thermal
Neutron Capture Cross Section at KURRI-LINAC
J. Hori et al. (26069) ...........................................................................................................
Experimental Study on Non-destructive Assay with a Pulsed Neutron Source
J. Hori et al. (26070) ...........................................................................................................

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3. Reactor Physics and Reactor Engineering
CO3-1
CO3-2

Development of In-reactor Observation System Using Cherenkov Light (VI)
T. Takeuchi et al. (26040) ·········································································· 108
Neutron Irradiation Effect of High-density MoO3 Pellets for Mo-99 Production (2)K. Nishikata et al. (26041) ········································································· 109

4. Material Science and Radiation Effects
CO4-1
CO4-2
CO4-3

Development of Radiation Tolerant Image Sensor with Field Emitter Array
Y. Gotoh et al. (26002) ············································································· 110
Sub-terahertz Absorption of Ionic Liquid
T. Awano et al. (26015) ············································································· 111
Generation of Circular Polarization using Linearly Polarized Coherent Transition Radiation
T. Takahashi et al. (26016) ········································································· 112v

CO4-4
CO4-5

CO4-6

Basic Study on Radiation-induced Luminescence from Natural Mineral
H. Fujita et al. (26027) ············································································· 113
Complex Structure of Ions Coordinated with Hydrophilic Polymer. 15. Applied Discussion
with Ionic Behavior in Hydrophobic Matrixes
A. Kawaguchi et al. (26052) ········································································ 114
Elucidation of Tritium Dynamics in Neutron Irradiated Tungsten
Y. Oya et al. (26063) ················································································· 115

5. Geochemistry and Environmental Science
CO5-1

CO5-2
CO5-3

CO5-4

CO5-5
CO5-6
CO5-7
CO5-8

CO5-9
CO5-10Central Diameters and Concentrations of Element in the Atmospheric Aerosols at
Sakai,Osaka
N. Ito et al. (26011) ·················································································
Study of Earth and Planetary Matters by Thermoluminescence
K. Ninagawa et al. (26024) ········································································
Evaluation of Redox Conditions at Dredged Trenches in Tokyo Bay by the Concentrationsof Elements in the Sediments
T. Yamagata et al. (26028) ·········································································
Characteristics of Synthetic Calcite Thermoluminescence Studied
Reconstruction of East Asia
N. Hasebe et al. (26029) ···········································································
Fission Track Ages of Sedimentary Rocks from Accretionary Belt in the Kii Peninsula
H. Ohira et al. (26036) ·············································································
Trace Amounts of Halogens (Cl, Br and I) in Manganese Nodule Reference Materials
M. Ebihara et al. (26043) ··········································································
Application of Neutron Activation Analysis to Micro Gram Scale of Solid Samples
S. Sekimoto et al. (26048) ·········································································
Probability Distribution of SEL Occurred on on-board Computer (OBC) Mounted on
Small-scale Satellite
S. Sekimoto et al. (26053) ·········································································
Instrumental Photon Activation Analysis of Geological and Cosmochemical Samples
N. Shirai et al. (26067) ·············································································
Decomposition of Perfluorooctane Sulfonate by Gamma Ray Irradiation
A. Hashiguchi et al. (26074) ·······································································

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6. Life Science and Medical Science
CO6-1
CO6-2

CO6-3
CO6-4
CO6-5

CO6-6

D-serine Acting as Competitive Inhibitor on Tryptophanase
A. Shimada et al. (26012) ···········································································
Study of Localization Estimation of Abasic Sites in DNA Irradiated with Ionizing
Radiation
K. Akamatsu et al. (26017) ··········································································The Effect of Boron Neutron Capture Therapy (BNCT) on Anti-tumor Immune Response
T. Suzuki et al. (26049) ··············································································
In situ Visualization of Boron in Plants Using Neutron Capture Radiography
M. Kobayashi et al. (26056) ········································································
Measurement of Transmittance Spectra of a Cryo-Sectioned Tissue of Brain Tumor
C6 Model in the Sub-Terahertz Reagion-II
N. Miyoshi et al. (26072) ············································································
Design and Synthesis of New Drugs for Boron Neutron Capture Therapy and Boron
Magnetic Resonance Imaging
S. Aoki et al. (26077) ················································································

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7. Neutron Capture Therapy
CO7-1

CO7-2

Evaluation of Boron-containig Rare Earth Oxides Nanoparticles as an Agent for
Boron Neutron Capture Therapy
T. Nagasaki et al. (26005) ·········································································· 132
In vivo Evaluation of Gd-DTPA-incorporated Calcium Phosphate
Nanoparticles as Neutron Capture Therapy Agent
N. Dewi et al. (26014) ·············································································· 133vi

CO7-3
CO7-4

CO7-5

CO7-6

Development of a Phantom for Estimation of Beam Quality in BNCTY. Sakurai et al. (26034) ············································································ 134
A Fundamental Experiment for the Measure Against the Activation of the Irradiation-room
Concrete at BNCT Facility
Y. Sakurai et al. (26035) ············································································ 135
Radiosensitizing Effect of Purinergic Antagonists on the Damage of Melanoma by
BNCT
M. Tsukimoto et al. (26061) ······································································· 136
Feasibility Study for Establishing QA Method for Hospital- and Reactor-based BNCTS. Nakamura et al. (26068) ········································································ 137

9. TRU and Nuclear Chemistry
CO9-1
CO9-2

Stability of Caprolactam Resin against γ-Ray Irradiation in HNO3
T. Nishida et al. (26013) ············································································ 138
Search for Ultraviolet Photons from Precipitated 229mTh Samples
Y. Yasuda et al. (26079) ············································································ 139

10. Health Physics and Waste Management
CO10-1

Study on the Behavior of Cs and Sr in Soil as Waste
M. Yoneda et al. (26075) ··········································································· 140

11. Accelerator Physics
CO11-1

CO11-2

Study of Intense Terahertz Light Source Based on Superimposing Backward
Coherent Diffraction Radiation
N. Sei et al. (26004) ················································································ 141
The XEP-e (eXtremely High Energy Plasma/ Particle Sensor for Electron) of the
ERG Satellite
N. Higashio et al. (26071) ········································································· 142

12. Others
CO12-1
CO12-2
CO12-3
CO12-4CO12-5

CO12-6

CO12-7CO12-8CO12-9Precise Determination of Br in ABS Resin by Instrumental Neutron Activation Analysis
T. Miura et al. (26008) ·············································································
Thickness and Density of Adsorbed Additive Layer onto Metal Surface
T. Hirayama et al. (26020) ·········································································
Characteristic Mesurement of Neutron Detector for Fukushima Debris
M. Kureta et al. (26022) ············································································
Evaluation of Multiwire-type Two-Dimensional Neutron Detector with Individual
Line Readout
K. Toh et al. (26042) ················································································Development of Neutron Resonance Densitometry for Nuclear Material Quantificationin Melted Fuel
F. Kitatani et al. (26044) ···········································································
Test of a Microcell Multi-Wire Proportional Chamber for a Muon-Electron Conversion
Search Experiment, DeeMe
H. Natori et al. (26046) ·············································································
Ethnographic Study of Nuclear Reactor
M. Takagaki et al. (26051) ·········································································
Effective Measures on Safety, Security, Hygiene and Disaster Prevention in Laboratories
T. Iimoto et al. (26054) ·············································································Development of New NiMo Neutron Mirror for Fundamental Physics
Y. Arimoto et al. (26059) ···········································································

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II. PUBLICATION LIST (April 2014 – March 2015) ······················································ 152vii

I. ANNUAL SUMMARY OF EXPERIMENTALRESEARCH ACTIVITIES1I-1. PROJECT RESEARCHES

2

PR1

Analyzing Tumor Microenvironment and Exploiting its Characteristics
for Controlling Malignant Solid Tumors and Distant Metastatic Potential
to decrease the number of lung metastases, and an acutehypoxia-releasing treatment such as the administration of
nicotinamide or bevacizumab may be promising for reducing numbers of lung metastases. Consequently,
BPA-BNCT in combination with nicotinamide and/or
bevacizumab treatment may show a little more potential
to reduce the number of metastases. Now, it has been
elucidated that control of the chronic hypoxia-rich Q cell
population in the primary solid tumor has the potential toimpact 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 to impact
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
newly-developed 10B-carriers based on the revealed findings on intratumor microenvironmental characteristics.

S. Masunaga
Research Reactor Institute, Kyoto University
BACKGROUNDS AND PURPOSES: 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 established experimental animal tumor cell lines. The presence of Q
cells is probably due, in part, to hypoxia and the depletion of nutrition in the tumor core, which is another consequence of poor vascular supply. As a result, Q cells are
viable and clonogenic, but stop cell division. In general,
radiation and many DNA-damaging chemotherapeutic
agents kill proliferating (P) tumor cells more efficiently
than Q tumor cells, resulting in many clonogenic Q cells
remaining following radiotherapy or chemotherapy.
Therefore, it is harder to control Q tumor cells than tocontrol P tumor cells, and many post-radiotherapy recurrent tumors result partly from the regrowth of Q tumor
cells that could not be killed by radiotherapy. 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 causesof post-chemotherapy recurrent tumors is an insufficient
dose distribution into the Q cell fractions.
With regard to boron neutron capture therapy(BNCT), with 10B-compounds, boronophenylalanine-10B(BPA) increased the sensitivity of the total cells to agreater extent than mercaptoundecahydrododecaborate10
B (BSH). However, the sensitivity of Q cells treatedwith BPA was lower than that in BSH-treated Q cells.
The difference in the sensitivity between the total and Q
cells was greater with 10B-compounds, especially with
BPA. These findings concerning the difference in sensitivity, including other recovery and reoxygenation following neutron irradiation after 10B-compound administration were mainly based on the fact that it is difficult
to deliver a therapeutic amount of 10B from 10B-carriers
throughout the target tumors, especially into intratumor
hypoxic cells with low uptake capacities.
Hypoxia is suggested to enhance metastasis by increasing genetic instability. Acute, but not chronic, hypoxia was reported to increase the number of macroscopic metastases in mouse lungs. We recently reported thesignificance of the injection of an acute hypoxia-releasing
agent, nicotinamide, into tumor-bearing mice as a combined treatment with -ray irradiation in terms of repressing lung metastasis. As the delivered total dose increased with irradiation, the number of macroscopic lungmetastases decreased reflecting the decrease in the number of clonogenically viable tumor cells in the primarytumor. The metastasis-repressing effect achieved througha reduction in the number of clonogenic tumor cells by
irradiation is much greater than that achieved by releasing tumor cells from acute hypoxia. On the other hand,more 10B from BPA than from BSH could be distributed
into the acute hypoxia-rich total tumor cell population,
resulting in a greater decrease in the number of highly
clonogenic P tumor cells with BPA-BNCT than with
BSH-BNCT and with neutron beam irradiation only.
BPA-BNCT rather than BSH-BNCT has some potential

採択課題番号 26P1

RESEARCH SUBJECTS:
The collaborators and allotted research subjects (ARS)
were organized as follows;
ARS-1 (26P1-1): Optimization of Radiation Therapy
Including BNCT in terms of the Effect on a Specific
Cell Fraction within a Solid Tumor and the Suppressing
Effect of Distant Metastasis. (S. Masunaga,et al.)ARS-2 (26P1-2): Development of Hypoxic Microenvironment-Oriented 10B-Carriers. (H. Nagasawa, et al.)
ARS-3 (26P1-3): Clarification of Mechanism of Radio-Resistance in Cancer Using Optical Imaging at Tissue Level. (H. Harada, et al.)
ARS-4 (26P1-4)*: Analysis of Radiation-Induced
Cell-Killing Effect in Neutron Capture Reaction. (R.
Hirayama, et al.)
ARS-5 (26P1-5): Transdermal Drug Delivery Systemusing Hyaluronan-Conjugated Liposomes as 10B-Carrier
in Boron Neutron Capture Therapy for Melanoma(S. Kasaoka, et al.)
ARS-6 (26P1-6): Evaluation of Inclusion Complex ofCarborane Modified Kojic Acid and Cyclodextrin as
10
B-Carrier in Boron Neutron Capture Therapy. (T. Nagasaki, et al.)
ARS-7 (26P1-7)*: Molecular Design and Synthesis andFunctional Evaluation of Anticancer and Molecular Targeting Agents. (Y. Uto, et al.)
ARS-8 (26P1-8)*: Analyzing Biological Effect of BNCT
from the Viewpoint of the Changes in Oxygenation Level. (H. Yasui, et al.)
ARS-9 (26P1-9): Analyses on the Responsiveness of
Malignant Tumors to BNCT. (M. Masutani, et al.)
ARS-10 (26P1-10): Assay for Tumor Cell Survival andTumor Growth Delay through Neutron Capture Reaction
according to the Changes in Intracellular Concentrations
within Solid Tumors of Newly- Developed 10B-Carriers.
(K. Nakai, et al.)
ARS-11 (26P1-11)*: Antitumor and MetastasisReppresing Effect of BNCT on Human Breast andPancreatic Cancer Cell Lines. (Y. Matsumoto, et al.)(* Due to the irregular and short operation period of ourreactor in 2014, the data could not be shown here.)

局所腫瘍制御と転移抑制を同時に目指す
治療法開発のためのがん微小環境解析とその応用（京大・原子炉）増永慎一郎
3

プロジェクトPR1-1Significance of Fractionated Thalidomide Administration Combined with γ-Ray
Irradiation from the Viewpoint of Local Tumor Response and Lung Metastasis

S. Masunaga1, Y. Sanada1, T. Moriwaki2, K. Tano1, Y.
Sakurai1, H. Tanaka1, M. Suzuki1, N. Kondo1, M. Narabayashi1, T. Watanabe1, Y. Nakagawa1, A. Maruhashi1
and K. Ono1

crosis factor from monocytes, and modulates other cytokine action. Thalidomide is racemic, and contains bothleft and right handed isomers in equal amounts: one enantiomer is effective against morning sickness, and theother is teratogenic. The enantiomers are converted toeach other at physiological conditions (pH = 7.0) in vivo.
That is, if a human is given D-thalidomide ((+)- or R-) or
L-thalidomide ((-)- or S-), both isomers can be found in
the serum. Hence, administering only one enantiomer
will not prevent the teratogenic effect in humans. It is
employed for the acute treatment of the cutaneous manifestations of moderate to severe erythema nodosum leprosum (ENL). Available data from in vitro studies andpreliminary clinical trials suggest that its immunologic
effects can vary substantially under different conditions,but may be related to suppression of excessive tumor
necrosis factor production and down-modulation of selected cell surface adhesion molecules involved in leukocyte migration [3].
As a cancer treatment, thalidomide was shown to inhibit basic fibroblast growth factor (bFGF) as well as
VEGF, two promoters of angiogenesis. It was reported tomeasure the modifications in the tumor environment early after an angiogenic treatment of thalidomide, with a
special focus on possible normalization of the tumor
vasculature that could be beneficial for radiotherapy [4].
Incidentally, angiogenesis also is critical during limb development of the foetus. Thalidomide directly inhibits
angiogenesis induced by bFGF or VEGF in vivo. In 2009,it was confirmed that loss of newly formed blood vessels
is the primary cause of thalidomide teratogenesis, andthat developing limbs are particularly susceptible becauseof their relatively immature, highly angiogenic vessel
network. Thus inhibition of angiogenesis is now thought
to be a main mechanism of its teratogenicity [3,5].
Conclusion: It was elucidated that control of the chronic
hypoxia-rich Q cell population in primary solid tumors
has the potential to impact the control of local tumors as awhole, while control of the acute hypoxia-rich total tumor
cell population has the potential to impact the control oflung metastases. Namely, in conventional radiotherapy,
daily fractionated administration of thalidomide combined with MTH is thought to have a great potential tocontrol both local solid tumors and lung metastases fromthe local tumors [6].
REFERENCES:[1] S. Masunaga, et al., Int J Hyperthermia 13 (1997)
401-411.
[2] S. Masunaga, et al., Clin Exp Metastasis 26 (2009)693-700.
[3] M. E. Franks, et al., Lancet 363 (2004) 1802-1811.
[4] R. Ansiaux, et al.,Clin Cancer Res 11 (2005) 743-750.
[5] C. Therapontos, et al., Proc Natl Acad Sci U S A 106(2009) 8573-8578.
[6] S. Masunaga et al., World J Oncol 5 (2014) 155-165.

1

Research Reactor Institute, Kyoto University
Faculty of Medicine, Kyoto University

2

INTRODUCTION: Thalidomide has been reported toinduce tumor blood vessel normalization in a mousemodel [8, 9]. Today, thalidomide is being mainly applied
as a treatment of certain cancers (multiple myeloma) andof a complication of leprosy. Here, using a readily metastasizing murine melanoma cell line, we tried to analyze the significance of combined treatment with thalidomide in radiotherapy with γ-rays in combination with anacute hypoxia-releasing agent nicotinamide or mild temperature hyperthermia (MTH), already shown to have thepotential to release tumor cells from diffusion-limited
chronic hypoxia [1, 2], in terms of local tumor response
and lung metastatic potential. Concerning the local tumor
response, the effect 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 insolid tumors.
Materials and Methods: B16-BL6 melanoma tumor-bearing C57BL/6 mice were continuously given
5-bromo-2’-deoxyuridine (BrdU) to label all P cells. The
tumor-bearing mice then received γ-ray irradiation after
thalidomide treatment through a single or two consecutive daily intraperitoneal administrations up to a total
dose of 400 mg/kg in combination with nicotinamide or
mild MTH. Immediately after the irradiation, cells fromsome tumors were isolated and incubated with a cytokinesis blocker. The responses of the Q and total (= P + Q)
cell populations were assessed based on the frequency of
micronuclei using immunofluorescence staining for BrdU.
In other tumor-bearing mice, 17 days after irradiation,
macroscopic lung metastases were enumerated.
Results: Thalidomide raised the sensitivity of the total
cell population more remarkably than Q cells in both single and daily administrations. Daily fractionated administration of thalidomide elevated the sensitivity of boththe total and Q cell populations, but especially the total
cell population, compared with single administration.
Daily administration, especially combined with MTH,
decreased the number of lung metastases.
Discussion: Thalidomide was originally introduced as a
non-barbiturate hypnotic, but withdrawn from the market
due to teratogenic effects. However, it has been reintroduced and used for a number of immunological and inflammatory disorders due to its immunosuppressive andanti-angiogenic activity. It inhibits release of tumor ne-4

PR1-2Development of Nucler-targeting Boron Carriers Based on the Chemistry of Direct
Cell-penetrating Pepducins

A. Isono1, K. Okuda1, T. Hirayama1, S. Masunaga2, and
H. Nagasawa1

was likely to be anchored on the plasma membrane but
could not be translocated into the cytosol. To evaluate thestructure activity relationship of the peptide sequence forcontrolling cellular distribution, we synthesized pepducins containing various peptides to conjugate with thecargo moiety.

1

Laboratory of Medicinal & Pharmaceutical Chemistry,
Gifu Pharmaceutical University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: For the success of boron neutron
capture therapy (BNCT), it is essential to selectively deliver sufficient amount of 10B atoms to tumor cells. To
achieve intracellular molecular targeting of drug delivery,
we focused on the direct cell-penetrating lipopeptides,
pepducins which were developed as allosteric modulators
of GPCRs[1]. By the study of fluorescence resonanceenergy transfer (FRET)-based imaging of pepducins, wedemonstrated that they penetrate directly into cells bytrans-membrane lipid translocation [2]. Accordingly, we
envisaged that the pepducin moiety may be exploitablefor intracellular deliver of membrane impermeable
molecules such as anionic boron claster, sodium borocaptate (BSH).
MOLECULAR DESIGN: As shown in Fig. 1, we designed new hybrid molecules comprising pepducin (Pep)
as a vehicle, and boron cluster (BS) attached with fluorescent dyes such as 7-hydroxycoumarin (Cou) andHoechst 33342 dye (Hoe) as a cargo; Pep-SS-BS-Cou
and Pep-SS-BS-Hoe. The cargo is supposed to be released into cytosol after reductive cleavage of the disulfide bond by intracellular glutathione when it is carried
into the cytosol.

We also synthesized Pep-SS-BSs by connecting of various pepducins to the boron cluster without any fluorophores. To quantify their intracellular boron concentration, ICP-MS analyses of nuclear and cytoplasmic extracts will be conducted.

RESULTS AND DISCUSSION: The lipidated peptides
were prepared by solid-phase synthesis and then combined with BSH and the corresponding fluorophorethrough an appropriate liker to afford the boron carriers(Fig. 2 and 3). We performed live cell imaging experiments using MCF-7 cells with the probes and confocal
microscopy. By the treatment with Pep-SS-BS-Cou, thefluorescence signal was localized on cell-membrane formore than 30 min, which suggested that the boron carrier

REFERENCES:[1] L. Covic et al., Proc. Natl. Acad. Sci. USA., 99(2002) 643–648.
[2] M. Tsuji et al., Org. Biomol. Chem., 11(2013),
3030-3037/.?E6! 261 A<,(4" 08  
C7

F*D>$>'G9B =%5+) :12;&F$ &3G#1-@

5PR1-3

Genetic Screening of Upstream Activators of Hypoxia-inducible Factor 1 for the
Devrlopment of Novel Anti-cancer Strategies

H. Harada1, S. Masunaga2, M.

Fig. 1

1

Department of Radiation Oncology and Image-applied
Therapy, Graduate School of Medicine, Kyoto University.
2
Research Reactor Institute, Kyoto University
INTRODUCTION:
Accumulating evidence has
shown that hypoxia-inducible factor 1 (HIF-1) plays critical roles in distant tumor metastases at multiple steps [1]and eventually causes death among cancer patients. Clinical studies have demonstrated consistent data that HIF-1
could be used as an adverse prognostic factor for not only
local tumor recurrence but also distant tumor metastasis
in cancer patients. These findings justify targeting HIF-1
for cancer therapies.
HIF-1, a heterodimeric transcription factor composed ofan -subunit (HIF-1) and a -subunit (HIF-1), is
known to become activate mainly through the stabilization of HIF-1 protein. Under normoxic conditions,prolyl-4-hydroxylases (PHDs) hydroxylate proline residues, P402 and P564, in the oxygen-dependent degradation domain (ODD domain) of HIF-1 in an oxygen-dependent manner. The hydroxylations trigger
polyubiquitilation and subsequent proteasomal degradation of HIF-1. On the contrary, HIF-1 becomes active
under hypoxic conditions because of the inactivation of
the hydroxylases, and then, interacts with its binding
partner, HIF-1. Resultant heterodimer, HIF-1, binds to
its cognate enhancer sequence, the hypoxia-responsive
element (HRE), and induces transcriptions of various
genes related to the escape from hypoxia (invasion andmetastasis of cancer cells) as well as the improvement ofoxygen-availability (angiogenesis) and adaptation of cellular metabolism to hypoxia (metabolic reprogramming).
In order to explore novel genes which are responsible
for the HIF-1-mediated tumor metastasis, we recently
established a new genetic screening method [2] andfound that overexpression of ubiquitin C-terminal hydrolase L1 (UCHL1) is responsible for the activation of
HIF-1. In the present study, we analyzed both the molecular mechanisms underlying the UCHL1-mediated activation of HIF-1 and the involvement of UCHL1-HIF-1
axis in distant tumor metastases.

A murine model of pulmonary metastasis demonstrated
that the forced expression of UCH-L1 facilitated tumor
metastases in a HIF-1-dependent manner (Fig. 2) [3].

Fig. 2On the other hand, silencing of the aberrantly expressed
UCH-L1 suppressed the metastatic tumor formation byinactivating HIF-1[3].
Moreover, we revealed that UCH-L1 expression levels
were associated with poor prognosis of patients withbreast and lung cancers (Fig. 3) [3].

Fig. 3DISCUSSIONS: Together, these results demonstratethat UCH-L1 functions in distant tumor metastasis as a
deubiquitinating enzyme for HIF-1, and thus, justify
exploiting it as a prognostic marker and therapeutic target
for individualization of cancer therapy.

EXPERIMENTS & RESULTS: We established stabletransfectants of HeLa cells with the UCHL1 expression
vector (HeLa/UCHL1) or its empty vector (HeLa/EV) [3].
We found that aberrant expression of UCH-L1 in cancer
cells abrogated von Hippel-Lindau-mediated ubiquitination of HIF-1, leading to the stabilization of HIF-1 andsubsequent activation of HIF-1 (Fig. 1) [3].

採択課題番号26 P1-3

REFERENCES (papers published from our lab):[1] Zhao T et al. Sci Rep. 4:3793. 2014.
[2] Zeng L et al. Oncogene. in press.
[3] Goto Y et al. Nature Communications. 6:6153. 2015.

低酸素誘導性因子1（HIF-1）を活性化する新規遺伝子の探索と機能解析、および局所腫瘍制御への展開（京大・院医）原田浩（京大・原子炉）増永慎一郎
6

プロジェクトPR1-4

Quantitative Detection of Metastasized B16BL6 Cells in Lung by Using
TaqMan RT-PCR Assay

T. Nagasaki, J. Kawaguchi, R. Kawasaki, M. Sakuramoto,
M. Kirihata1, Y. Hattori1, S. Masunaga2 and Y. Sakurai2

tion (Q-PCR) was performed according to the manufac(Roche) and Q-PCR was run in a STRAGENE Mx3000P
using the following program:. Primers and probe were
AGC ACC TGG AAC CACGAG GGC GTTATC TATGT GTA GT 3probe: 5'Hex-CAC TAC AAA
AGT TGT GGG TAC TAC ACC TG-BHQ-1-3'.

Graduate School of Engineering, Osaka City University
1
BNCT Research Center, Osaka Prefecture University,
2
Research Reactor Institute, Kyoto University
INTRODUCTION:
Although melanoma boron neutron capture therapy (BNCT) with L-10B-p-boronophenyl
alanine has been treated for melanoma patient, the enhancement of 10B accumulation in melanoma cells would
lead to improved efficacy of malignant melanoma BNCT.
Recently, we have evaluated the inclusion complex of
kojic acid-appended carborane (CKA) with hydroxypropyl- -cyclodextrin (HP- -CD) as a novel boron agent for
BNCT toward melanoma. CKA/HP- -CD complex
showed melanoma cells selectivity, unique nuclear localization, and high tumor-suppression effect on BNCT towardmelanoma-bearing
mice.
Furthermore,
CKA/HP- -CD complex was found to be the potent inhibitor of hypoxia-induced HIF-1 and to have a strong
effect on tumor metastasis [1]. Herein, in order to evaluate quantitatively metastasis-suppression, TaqMan
RT-PCR assay of melanoma gene GP100 was carried out
toward melanoma B16BL6 cells metastasis from thighsubcutaneous to lung in melanoma-bearing mice [2].

Fig.1 Relative mRNA expression of melanoma gene
GP100 in lungs.

RESULTS AND DISCUSSION: GP100 is highly
expressed in melanoma B16BL6 cells, but not to any
substantial degree in normal tissues. GP100 expression
exceeded background levels when at least 5 103 B16BL6
cells are contained in metastasized tissue. In order toquntify the increase of metastasized B16BL6 cells, lungs
were collected 1, 3, 7, or 14 days post tumor implantation.
On day 7 increase of GP100 expression reached a levelof about 100 times the lowest point (Fig. 1).
TaqMan RT-PCR Assay toward GP100 is potent toestimate quantitatively the metastasis of melanoma cells
to lung. The quantitative evaluation of metastasis-suppression effect of CKA/HP- -CD complex is proceeding in our laboratory.

Structure of CKA/HP- -CD

EXPERIMENTS: B16BL6 cells (2.5 1012 cells) were
implanted into thigh subcutaneous. Mice were euthanized
and lung and spleen were isolated and snap frozen in liquid nitrogen before being stored at Total RNA wasextracted using NucleoSpinRNA Kit (Takara). Total
RNA concentration and purity were measured using
NanoDrop 2000c Spectrometer (Thermo Scientific).
Subsequently, cDNA synthesis was performed by using
PrimeScriptTM RT reagent Kit (Perfect Real Time)(Takara). Quantitative real time polymerase chain reac-

REFERENCES:[1] K. Shimizu et al., Bioorg. Med. Chem. Lett., 20(2010) 1453-1456.
[2] M. R. Sorensen et al., PLoS One., 9 (2001)
e87831.

メラノーマ中性子捕捉療法への適応を目指した薬物送達システムに関する研究7

PR1-5

Response of Tumor Cells to BNCTS. Imamichi1, T. Itoh1,2, S. Kikuhara1,2, H. Fujimori1, A.
Sato3, T. Hirai1,4, S. Masunaga5 and M. Masutani1,6

minescence dosimeter. These physical radiation doses
were measured with the kind help of Drs. Yoshinori Sakurai and Hiroki Tanaka of KUR.

1

Division of Chemotherapy and Clinical Research, National Cancer Center Research Institute, 2Faculty of Industrial Science and Technology, Tokyo University of
Science, 3Faculty of Pharmaceutical Sciences, Tokyo
University of Science, 4Department of Radiation Oncology, Juntendo University Faculty of Medicine, 5 Research
Reactor Institute, Kyoto University, 6Department ofFrontier Life Sciences, Nagasaki University Graduate
School of Biomedical Sciences

RESULTS:
Fig. 1. The physical dose measurement.
Themeasuredresults of total
physicaldose,
neutronandgamma ray dosewere shown in
Fig. 1 and confirmed that thedose estimation
was in the expected
range.
Twenty-four hrs
after 24 Gy-eq
irradiation, SAScells showed thecleavageof
PARP1, caspase-9 and caspase-3, suggesting that apoptosis started to occur. Meanwhile, the low levels of necroticcleavage pattern of PARP1 were also observed, implyingthat necrotic cell death is also involved after BNCR. The
isolated RNA 6 and 24 hrs after irradiation was evaluatedby electrophoresis and RT-PCR. As shown in Fig. 2, theexpression levels of PARP1 and GUSB were not different
among the irradiation conditions, confirming the qualityof RNA. In the microarray analysis, we found that theexpression of the genes related to cell death, transcription,and inflammatory and immune responses was augmented
after BNCR and the further evaluation is ongoing.
By proteome analysis, proteins involved in the vesicle
regulation, mRNA processing, transcription were observedwithchanges
after
BNCR and being
studiedfurther.
Theobservationsuggests that dynamic changes in cellular responses could
be induced after BNCR reaction at an early phase. SAS
xenograft model in nude mice was also set up, and theboron concentration in the blood and tissues was measured. Using the experimental system, the genes and proteins associated with BNCR response will be further elucidated.

INTRODUCTION: Tumors are consisted of heterogenous populations of cells, including hypoxic cells,
cancer stem cells and differentiating cells. These populations affect the consequence of the boron neutron capture
therapy (BNCT) [1]. Boron neutron capture reaction(BNCR) causes extensive DNA double strand breaks andmicronuclei formation has been used to estimate the levelof DNA damage induced by BNCR [2]. In rat xenograftmodel, BNCR caused the up-regulation of H2AX and
HMGB1, then induction of poly(ADP-ribose) [3]. The
cell death process and the factors affecting tumor cellkilling, side effects and effectiveness of BNCT are notfully understood. To elucidate the cell death process after
BNCR, we have taken approaches of comprehensive
analysis of the tumor cells by using transcriptome andproteome analysis.
EXPERIMENTS: Human oral squamous cancer SAS
cells [1] was used for the comprehensive analysis withandproteome
analysis.
transcriptome
10
B-boronophenylalanine (10B-BPA)-fructose solution
was prepared as described previously [4]. SAS cell was
suspended and incubated 2 h with or without 25 ppm of
10
B-BPA as previously reported [3]. After neutron-beamirradiation operated at 1 MW, cells were inoculated forcolony formation, RNA and protein preparation. To analyze the early response of cancer cells, RNA and protein
were prepared 6 and 24 hrs after irradiation at the supposal doses of 4 Gy-eq and 24 Gy-eq conditions.
For mouse xenograft model, male BALB/c-nu/nu
mice were used and SAS cells were injected subcutaneously into left legs of the mice. 10B-BPA at the dose of
250 mg/kg bodyweight was intraperitoneally injected 1 h
before irradiation operated at 1 MW. Tumors, tissues, andblood were sampled for the analysis of early responses
after irradiation. The animal studies were performed inaccordance with the relevant laws and institutional guidelines of KUR and NCC. 10B concentration was measured by prompt-gamma ray analysis (PGA). Thermal
neutron fluence was measured with gold foils activation
analysis. Gamma-ray dose was measured with thermalu-

採択課題番号 26P1-9

REFERENCES:[1] Masunaga et al, Jpn. J. Cancer Res., 93(12) (2002)
1366-77.
[2] Kinashi et al, Radiat. Oncol., 5;6 (2011) 106.
[3] M. Masutani et al, Appl. Radiat Isot.88 (2014) 104-8.
[4] Yoshino et al, Strahlen. Onkol., 165: (1998) 127-12ホウ素中性子捕捉療法に対する腫瘍応答機構の分析と奏効バイオマーカーの探索

プロジェクト(京大・原子炉）増永慎一郎（国立がん研究センター）益谷美都子、今道祥二、佐藤聡、伊藤祐
菊原颯太、平井崇久、藤森浩彰

8PR1-6

Additive effect of Gadolinium to cell survival analysis
for neutron capture therapy

K. Nakai1, F. Yoshida1, T. Kurita1, Y. Yamamoto1, M.
Shirakawa2, T. Yamamoto1, H. Tanaka3, Y. Sakurai3, S.
Masunaga3

RESULTS: As shown in Fig. 1, Radiation-related
damage significantly increased with the increase of gadolinium concentration. When 5 ppm of Gd-DTPA wasadded to 40 ppm of BPA in C6 cells, the additive effectwas obtaine. In radiosensitive V79 cells the survival fraction dramatically decreased after irradiation and was
lower than 10% at boron concentration of 40ppm.

1

Department of Nueurosurgery ,Faculty of Medicine,
University of Tsukuba
2
Department of Pharmaceutical Sciences,International
University of Health and Welfare
3
Research Reactor Institute, Kyoto University
INTRODUCTION: In neutron capture therapy; thetherapeutic effect of a boron compound is based on alphaparticle production in a 10B(n, α) 7Li reaction, while agadolinium compound effect is based on producing
gamma rays derived from a 157Gd(n, γ) reaction[1,2].
Gadolinium containing agents has been used for contrast
enhance of MRI scan, and are commercially available as
pharmaceutical products.
If gadolinium is administered simultaneously with boron and irradiated with neutrons, it might become asource of additional local gamma rays, which correspondwith recent BNCT clinical trial protocol for glioblastoma.
We analyzed the additive effect of gadolinium on boron
based neutron capture reaction.
Materials and Methods:
Boron and Gadolinium compounds
p-boronophenylalanine (BPA) was obtained from Interpharma Praha (Praha, Czech Republic). Gd-DTPA(Magnevist) was purchased from Shering (Berlin, Germany). BPA and fructose ware dissolved and prepared aspreviously described. Briefly, BPA was converted to
BPA-fructose complex by mixing BPA and fructose in
NaOH. The pH was adjusted to 7.4 with HCl. Dissolution
solvent for Gd-DTPA was cell culture medium.
Cell lines; C6 rat glioma cell lines and V79 Chinese
hamster cell lines were maintained in Eagle’s Minimum
Essential Medium (MEM; Sigma-Aldrich), supplemented
with 10% fetal bovine serum.
Colony Formation Assay ;V79 cells and C6 cells after
exposition with the compounds were irradiated with neutron mixed beam for 90 min at the Kyoto University Research Reactor (KUR). We use the combination of BPA(0, 10, 20, 40 Bu µµg/mL) and Gd-DTPA (0, 0.5, 5, 10
Gdµg/mL) with 104 of cells of each line. The number ofcells was sufficient to produce 20-100 colonies at eachboron concentration. After 7days of incubation, the plates
were stained with 0.25 % methylene blue in 90 % ethanol.
Colonies of more than 50 cells were counted.

Fig. 1. Influence of Gd on BNCT in C6 (upper), V79(lower) cell lines. The symbols ◆ show the control(BPA only); ■ show the result of additional 0.5 ppm of
Gd; ▲ show the result of additional 5 ppm of Gd and× show the result of additional 10 ppm of Gd.

REFERENCES:[1] A. Matsumura et al.,J Exp Clin Cancer Res. (2005)24.
[2] Shikata F., et al. Eur. J. Pharm. Biopharm(2002)53.

	
 採択課題番号26P1-10	
 新規ホウ素化合物等を用いた中性子捕捉反応による細胞生存試験および腫瘍増殖抑制効果	 	 	  	  プロジェクト	
  （筑波大・医）中井	
  啓、吉田文代、山本陽平、高	
  振宇、
栗田	
  正（国際医療大・薬）白川	  真（京大・原子炉）田中浩基、櫻井良憲、増永慎一郎	
 
9

PR2

Direct observation of the proton or protonation in a protein moleculeby neutron and high resolution X-ray joint analysis

Y.Morimoto
Research Reactor Institute, Kyoto University

coli, enter into the 20S particle by the AFM. The in situ
detection of the degradation will make clear in vivo
mechanism in the living cell.
Other research of the structure analyses, catalase fro mbovine liver has been crystallized in deuteriu m solution.
Diffract ion data of the Spring-8 showed clear electron
densities at an active site, heme, and water passing tunnel(following figure). Ho wever, the resolution 2.5 Å is notenough to determine hydrogen atoms.

OBJ ECTIVES: Protein sciences are accelerated withuse of a neutron and an X-ray beam to clarify the tertiaryand quaternary structural information. Proton and/or protonation of the amino acids in the protein molecule affecta chemical react ion in the biological macro mo lecule,neutron is well useful to isolate findings of such reaction
mechanis ms and can determine a precise position androles of hydrogen or protonation in active amino acids.
Drugs, as reagents, anti-cancer compounds, play important roles in a host-protein molecu le with electrons or
protons, hydrogen (deuterium) ato ms should be determined clearly to design a compound molecule. X-ray
analysis is good method to find a whole mo lecule andneutron is sensitive and selective to hydrogen (deuterium),the both complementary usage or joint refinement of theprotein mo lecule is very powerful technique to analyze aprecise reaction mechanism with atomic resolution.
I have called for members to carry out the examinationof this purpose.
(1) Structural investigation of the 20S/26S Proteasome in
the highly structural organization, Y.Morimoto(2) Improved Techniques for Neutron Biology. T.Chatke(3) Proteolytic en zy mes derived fro m NephilaClavata.
Y.Hidaka

An ultra-high resolution (~0.9A) analysis of the lys ozy me crystallized under deuteriu m solution has been investigated by thermal turbulence refinement of carbon
and/or nitrogen atoms with use of the Photon Factorydata.
26P2-2
T. Chatake, S. Fujiwara, I. Tanaka, Y. Yanagisawa reported “Development of Improved Techniques for Neutron Bio logy” of the result for the three interesting
waorks. The first is a newly structure determination
method of the neutron crystallography by use of a H/Dcontrast density mapping, like to be a solvent flatteningof the X-ray determination. The second describes a fully
deuterated protein production method by overexpression
system, and mod ification of a cu ltivation and purificationof the kinase. The last is interesting view point on theneutron scattering or diffraction, by use of dynamic
polarization technique for a neutron biology.

RESULTS:
26P2-1
T. Murakami, M. Unno, I. Hisatome, K.Hosokawa, H.
Yamaguchi and Y. Morimoto reported “Degradation control and structural motion of the 20S/ 26S proteasome
elucidated by genetic mutation and atomic force microscope”. A newly inhibitor of the 20S proteasome and its
complex is described. Since the wild-type 20S proteasome has gradual decrease against drug concentration,
Y170A, Y170L and Y170F has no clear decreasing. Drug
A has an aromatic ring in its structure, the aromatic ringinteracts the Y(tyr) ring but F(phe) has also a ring stru cture. 26S whole structure has been investigated by the
AFM. The 26S has two large co mponents (19S) at thebothe ends of 20S particle. The AFM images show thesize of the whole part icle o f 26S, but a single-capped
particles are also observed with self-rotating images. We
have tried to detect when a substrate molecule, 6 x His
tagged protein generated by expression system of the E
採択課題番号 26P2

26P2-3
Y. Hidaka , M. Fujiwara, T. Nakanishi, S. Sh imamoto, andM.
Miyazawa
reported“Identificat ion
andcharacterization of p roteolytic enzy mes derived fro m
NephilaClavata” focusing to the spider protease digestting amyloid fibers including pathogenic -amyloid,such as amylo id fibrils, associated with the developmentof Alzheimer's disease. The N-terminal amino acid sequence of spider protease was determined by Ed man
degradation. Spider genes were amp lified using generating primers, base on the N-terminal amino acid sequence,by RT-PCR and cloned into pBR-SKII(-).The cloning of
spider protease genes is in progress.

蛋白質分子内のプロトン・プロトン化の直接観察（京大・原子炉）森本幸生

10

プロジェクトPR2-1

Degradation control and structural motion of the 20S/26S proteasome
elucidated by genetic mutation and atomic force microscope

T.Murakami1, M.Unno2, I.Hisatome3, K.Hosokawa1,
H.Yamaguchi1 and Y.Morimoto

Binding site of inhibitor is closed to Tyr170 and Thr1 ofthe β5 subunit. It is considered that an aromatic ring of
the inhibitor interacts with Y170 by ring-stacking force.
Genetic mutation for Y170 would have activities becauseof a lack of aromatic ring in the amino acid residue in the
Ala and Leu, binding ability of the inhibitor might be lost.
Typical activity assay for wild-type 20S shows reduction(Fig.1), but its concentration is slightly high rather than aclinical usage.

Research Reactor Institute, Kyoto University
School of Science and Technology,
Kwansei Gakuin University
2
Graduate School of Science and Engineering,
Ibaraki University
3
Institute of Regenerative Medicine and Biofunction,
Tottori University
1

INTRODUCTION: Proteasomes are the multicatalytic
protein complexes with huge molecular weight. It is wellknown that the ubiquitin proteasome system plays animportant role in regulated proteolysis. Proteasomes are
known to act as antigen-processing enzymes responsible
for the generation of peptide ligands presented by major
histocompatibility complex (MHC) class I molecules. In
the 20S proteasome each of 1, 2 and 5  subunits has
different enzyme activities; 1 has caspase-, 2 tryptic- and5 chymotryptic-like activities. It was found recently that
inhibition of 20S proteasome activity resulted in decrease
and disappearance of cancer cells. Since weak interactionof compounds to active amino acid residues we found,processing or degradation assay have been clarified byuse of genetic mutations of the yeast 20S proteasome.
The whole particle, 26S proteasome, including such 20S
core is very important in the actual living cell for a degradation or stabilization on the cell circulation. Especially,a motion or behavior of the 26S proteasome when a regulatory particles bound should be clarified at atomic- or
nano-scale resolution, we have tried to visualize such
behavior as a motion capture of the atomic force microscopy (AFM) technique.

The AFM measurement shows whole structure of the 26Sparticle, and analyses of resultant images describe ashape and size, and also a structural motion (Fig.2).

Fig.2a shows a double-capped whole 26S particle composed of central 20S and the both ends (19S regulatory
particles). Those ends, however, are same direction likesquare brackets. Fig.2b-e shows a single-capped 26S, itmeans that preparation of the 26S is insufficient or scarceof ATP. Fig.2b to 2e is spent six seconds, in the meantime
19S part seems like to bow twice. In this case, since a
preparation buffer includes no ATP reagents, it is interesting in such a motion by random movement or biologically functional changes. On the other hand the images
are also considered the single-capped particle to be rotated in a solution, physical fixation of the 20S core to abasal plate should be required and the subject for a future
study. This work was supported by a grants-in-aid for the
Customer Care Plan Foundation (YM). The synchrotron
radiation experiments were conducted under the approvals 2013AB6856, 2014A1855 and 2014AB6956, ofSPring-8.

EXPERIMENTS:
Genetic modification such as
Y170A, Y170L and Y170F are succeeded in the 5 subunit of the yeast. Wild and mutant cells were homogenizedby glass beads and the crude extracts were purified by
M2 affinity chromatography and Mono-Q anion exchange one. When the 26S particle was isolated,gel-filtration chromatography was continuously appliedwith a buffer solution including ATP. Isolated 20S proteasome was concentrated by ultrafiltration, andco-crystallized with small ligand and inhibitor molecules.
AFM measurements of the 26S particle were carried out
in the Research Institute of Biomolecule Metrology inTsukuba.
RESULTS: The electron densities with a resolution of
2.85Å have been observed at the active site in the β-ring.

採択課題番号 26P2-1 酵母プロテアソームの高次構造形成と活性動作機構の解明 プロジェクト（関学大理工）村上琢人、細川桂一、山口宏、（茨城大理工）海野昌喜、（鳥取大医）久留一郎（京大・原子炉）森本幸生

11

Development of Improved Techniques for Neutron Biology

PR2-2

T. Chatake, S. Fujiwara1, I. Tanaka2, Y. Yanagisawa3

EXPERIMENTS and RESULTS:(1) A new technique for neutron structure determination.
In the previous study, D2O- and H2O- solvent crystals ofbovine pancreatic ribonuclease A were prepared (21P9-6),
and their neutron diffraction images were collected at
BIX-3 at JRR-3M (JAEA). In this fiscal year, The D/Hcontrast neutron map was calculated in real space, anddiscrete peaks could be observed at the positions of D/Hexchangeable atoms inside and outside of the protein [1].
The detailed investigation of the hydration of the protein
is in progress.

Research Reactor Institute, Kyoto University
1
Japan Atomic Energy Agency
2
Faculty of Engineering, Ibaraki University
3
Fuculty of Pharmacy, Chiba Institute of Science
INTRODUCTION: The neutron diffraction technique isundoubtedly one of important methods for elucidating
behavior of hydrogen atoms in biological systems, aswell as neutron scattering technique. Nevertheless, neutron diffraction analysis is not a popular method forstructural biology yet, in comparison to a large number of
X-ray diffraction analyses. The main reason of the limitation of neutron diffraction experiments is, of course, thelower flux of neutron beam against those of X-ray
sources. On the other hand, several technical problems,
which derive from to the lack of experimental experience,
become obstacles for this forefront science. In this project,
the following three themes were studied for neutron
structural biology.

(2) An improved technique for production of deuterated
biomolecule in bacteria.
In the previous study, nattokinase (NK) and menaquinone-7 (MK-7) from Bacillus subtilis natto were purified,
and the non-hydrogen structure of NK was determined by
X-ray diffraction technique [2]. In addition, D2O-resist
Bacillus subtilis natto was obtained by successive cultivation in D2O medium [3] (21P9-3, 22P6-2, 23P2-2,3 and24P5-4). NK and MK-7 are expected for good samples
for neutron biology, NK neutron crystallography, MK-7
neutron small angle scattering. In order to perform theseneutron experiments, deuterated NK and MK were necessary. In this fiscal year, the improvement of the amountof production was tried. The temperature of the cultivation was estimated to be 42 degree. In addition, hipolypeptone was not good for the cultivation, although hipolypeptone was superior to polypeptone in the cultivationof native Bacillus subtilis natto in H2O medium.

(1) A new technique for neutron structure determination.
(Fujiwara and Chatake).
A new technique for the deuterium/hydrogen (D/H)
contrast map (the neutron scattering length of D and H
atoms is largely different.) in neutron macromolecular
crystallography is in developing by us. Our results suggested that this type of neutron map had advantages on
the neutron structure determinations.
(2) An improved technique for production of deuterated
biomolecule in bacteria.
(Yanagisawa and Chatake)
Deuteration of protein has been the important technique for neutron biology, and the most popular method is
the overexpression of the target protein using geneticallyengineered E. coli. Meanwhile, in food industry, a considerable number of materials and supplements are produced in native bacteria. In this project, the protocols of
producing deuterated biomacromolecules in Bacillus subtilis natto have been developed and improved.

(3) The basic research of the application of dynamic neutron polarization (DNP) for neutron protein crystallography (NPC).
2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) is a kindof radical, which is widely used for DNP. In the previous
study, TEMPO was introduced in crystals of hen egg
white lysozyme, and was confirmed in physicochemical
method [4]. Recently, death-associated protein kinase(DAPK) was expressed and purified for neutron crystallography, and its X-ray structure was reported [5].

(3) The basic research of the application of dynamic neutron polarization (DNP) for neutron protein crystallography (NPC).
(Tanaka and Chatake)
DNP is the sophisticated technique in neutron science. In
DNP, polarized neutron alters its coherent and incoherent
scattering depending on the nuclear spin of the polarizedhydrogen. DNP is already applied for neutron scattering
except biomolecules. In this project, the basic experiments essential for DNP were carried out.

REFERENCES:[1] T. Chatake, S. Fujiwara, to be published.
[2] Y. Yanagisawa et al., Acta Crystallogr. F66 (2010)
F66 (2010) 1670-1673.
[3] Yanagisawa, Y. et al., J. Synchrotron Rad. 20 (2013)875-879.
[4] Tanaka, I. et al., J. Synchrotron Rad. 20 (2013)958-61.
[5] Yamaguchi, A. et al., JPS Conference Proceedings, inpress.

プロジェクト

26P2-212

PR2-3 Identification and characterization of proteolytic enzymes derived from NephilaClavata
Y. Hidaka1, M. Fujiwara1, T. Nakanishi1, S. Shimamoto1,
and M. Miyazawa2

electrical stimulation using a micropipet. The extracts
were applied to SDS-PAGE and the enzymatic activity ofthe protein bands was estimated by a casein protease assay [4]. Two protein bands showed protease activities
and their molecular weights were estimated to be approximately 21.9 and 19.5 kDa, based on the SDS-PAGE
analysis [1]. To characterize the enzymes, FLGLPAKADA-NH2 and SIFKTLRTIA-NH2 were synthesized asmodel peptide substrates and treated with the crude spider protease. The results indicated that the spider protease can be classified as a Ca2+-dependent carboxypeptidase.
To further characterize the spider protease, theN-terminal amino acid sequence was determined by Edman degradation using blotted protein bands on PVDF
membrane after SDS-PAGE separation. The results suggested the N-terminal amino acid sequence of the spider
protease. Based on the amino acid sequence, generated
primers for the gene cloning of the protease were prepared and RT-PCR was performed using mRNA’s fromgut cells of Nephila Clavata. Three clones were isolated
and provided second PCR to produce cDNA’s of spider
proteases. The purified candidate cDNA’s were inserted
pBluescript SKII(-) and sequence analyses were performed. However, the sequence analysis of the cloned
spider protease gene revealed that the cloned genes were
non-specifically amplified during RT-PCR.
In conclusion, Spider protease was extracted fromits digestive fluid and exhibited strong protease activity.
The protease can be classified as a Ca2+-dependent carboxypeptidase, based on the results of protease inhibition
assays. The N-terminal amino acid sequence of spider
protease was determined by Edman degradation. Spider
genes were amplified using generating primers, base on
the N-terminal amino acid sequence, by RT-PCR andcloned into pBR-SKII(-). However, DNA sequence analysis indicated that the cloned DNA was non-specifically
amplified during RT-PCR. The cloning of spider proteasegenes is in progress.

1

Graduate School of Science and Engineering Kinki
University
2
National Institute of Agrobiological Sciences
INTRODUCTION: Spiders hunt insects using a web
net. The fact that they eat them without chewing, indicatethat spiders possesses highly efficient digestive enzymes[1]. Our previous studies suggest that spider’s proteolytic
enzymes are able to digest synthetic spider dragline amyloid fibers [2,3]. Thus, the spider protease has the potential ability to digest amyloid fibers including pathogenic
-amyloid, such as amyloid fibrils, that are associatedwith the development of Alzheimer's disease [1]. Therefore, we purified, identified, and characterized the enzymes derived from Nephila Clavata. The sequence
analyses of the blotted protein on a PVDF membrane
showed N-terminal amino acid residues. Based on thissequence information, we tried to clone the protease
gene.
EXPERIMENTS: The spiders (Nephila Clavata) werecollected in the field of Kyoto University Research Reactor Institute and the spider saliva including proteolytic
enzymes was obtained from Nephila Clavata (50 heads)
by electrical stimulation. The extracts were stored in a
deep freezer until use.
Casein protease assay [4] of the crude spider enzymes
was performed, as previously reported [1]. Peptide substrates for the assay of the protease activity of spider enzymes were chemically synthesized by the Boc solid
phase method, treated with hydrogen fluoride, and purified by reversed phase HPLC [1, 4].
The N-terminal protein sequence was determined by the
Edman degradation. First, the spider saliva was applied to
SDS-PAGE, and the proteins bands were electricallytransferred to a PVDF membrane. The electro-blotting of
spider proteases was performed using the semi-dry blotting method then applied to then-terminal sequence analysis
Based on the N-terminal sequence, we prepared generated primers for the gene cloning and RT-PCR was performed using mRNA’s from gut cells of Nephila Clavata.

REFERENCES:[1] M. Fujiwara et al., Peptide Science, 2013, 447-448(2014).
[2] S. Zheng, et al., Appl. Spectrosc., 43, 1269-1272(1989).
[3] Y. Hidaka, et al., Biopolymers, 96, 222-227 (2011).
[4] C. Dicko, et al., Biochemistry, 43, 1269-1272 (2004).

RESULTS: Spider’s digestive fluid that includes proteolytic enzymes was obtained from Nephila Clavata by

採択課題番号26P2-3
ジョロウグモ由来消化酵素の機能評価
プロジェクト（近大・総合理工学研究科）日高雄二、藤原充俊、中西建祥、島本 茂（農生）宮澤光博（京大・原子炉）森本幸生
13

PR3

Project Research on the New Applicant Development using the Characteristics of
the Particles from the Neutron Capture Reaction

and biological effects (cell killing and induction of
DNA double strand breaks (DNA-dsb) using humanglioblastoma cells, A172 and T98G. A172 are wild
type of p53, and T98G cells are mutant type.
The results showed that difference of radiation sensitivity between A172 and T98G was decreased by
BPA addition irradiation of neutron beam. These
results indicate that the difference between the radiation sensitivity was observed between the T98G
cells and A172 cells boron neutron capture reaction.
Interestingly, it was reduced with BPA where theirradiation mainly depends on the particle radiation
emitted by BNCR (Boron Neutron Capture Reaction). This result suggests that BNCT is an effective
treatment with glioblastoma that can reduce the difference of radio sensitivity by p53 functional status.
PRS-3 compared the different damage effects onplants between BNCR and 60Coγ-ray. To determine
the effectiveness of BNCR for plant mutagenesis at
irradiation of dry seeds, two-row-barley was easily
used because of its compact size of the seeds andhigher mutation rate. The dry seeds of Hordeumvulgare cv.Hayadori were immersed in different
concentrations of 10B-enrichedp-boronophenylalanine (BPA) for 24hours, and all
the materials were irradiated with thermal neutronfor 120 minutes in the Kyoto University Research
Reactor (KUR).60Coγ-ray irradiations were also
carried out on the „Hayadori‟ dry seeds in the different doses using the Kyoto University‟s 60Coγ-ray
irradiation facility. They found out that thesemi-lethality dose (LD50) and RD50in the reduced
rate of 4-week-seedlingswas 74.2μM BPA. The
469μM value was transformed to the total physicaldoses as17.98 Gy, and the 74.2μM as 11.2Gy byusing the transformation equation.
PRS-4 developed boron tracedrugs with their “ondemand” traceability and their physical force forneutron dynamic therapy (NDT). The boron tracedrug, UTX-51 was studied that their dynamic,
beyond chemical, effects when acquired by weak
thermal neutron irradiation of glycated BSA as amodel of advanced glycation end-products (AGEs),
which is linked to diabetes and aged diseases. They
found that all doses of the boron tracedrug UTX-51
caused destructive dynamic damage against
Gly-BSA during thermal neutron irradiation, suggesting boron tracedrugs could be used as dynamic
drugs for NDT targeted glycated proteins, such as
Gly-BSA, for serum protein-quality-control treatmet of AGEs-related diseases.

Y. Kinashi
Research Reactor Institute, Kyoto University
Objectives and Participating Research Subjects
In this project, we are intending to develop the new
application using the characteristics of the particles
from the neutron capture reaction.
PRS-1 Analysis of mutation in the mammalian cells
induced by BNCR (boron neutron capture reaction)( Y. Kinashi et al. )PRS-2 Analysis of double strand breaks in the
mammalian cells induced by BNCR
( S.Takahashi et al. )PRS-3 Application of BNCR to plant tissue culture
for mutation breeding( T.Morikawa et al.)PRS-4 Development of pharmacokinetic using boron
trace drugs( H. Hori et al. )Main Results and Contents
PRS-1 inspected whether ascorbic acid was effective in protection of the mutation induction of neutron radiation beam used for BNCT in Kyoto University Research Reactor (KUR). The mutagenicity
measured by the frequency of mutations induced byneutron irradiation with or without boron compound.
The HPRT locus was examined in Chinese hamster
ovary (CHO) cells irradiated with neutrons of KUR.
High dose rate neutron irradiation was 0.2Gy/min
with 5MW of KUR, and low dose rate neutron irradiation was 0.04Gy/min with 1MW of KUR. They
investigated that dose rate effect is exist neutron
irradiation in BNCT. Ascorbic acid treatment reduced mutation induction following neutron radiation. In neutron irradiation at high dose rate with
BPA, the mutation induction was controlled mosteffectively. This result suggests that the ascorbate
may protect the mutagenic effects of BNCT on thenormal tissue cells that take up the low dose of boron compounds. They confirmed that the ascorbic
acid was effective in protection of the mutation induction of neutron radiation beam used for BNCT.
PRS-2 investigated the most important biologicaleffects, i.e., DNA damages, after the irradiation withheavy ion particles from BNCR and neutron beam.
They advanced research related to the status of p53

採択課題番号 26P3 硼素中性子捕獲反応(BNCR)誘発粒子線の特性利用の新展開（京大・原子炉）木梨 友子
㻝㻠

プロジェクトPR3-1 The effect of ascorbic acid on the HPRT mutation induction after the neutron irradiation
Y. Kinashi1, K. Ono1, S.Takahashi1
1Research Reactor Institute, Kyoto University

INTRODUCTION: We have previously reported
the increased mutagenicity of thermal neutrons and thedose rate effect of the neutron radiation beam [1].
Clinically, the mutagenic effects of BNCT on the normal tissue cells that do not take up the boron compounds may cause the genetic instability and second
cancer decade years after BNCT. In this study, we inspected whether ascorbic acid was effective in protection of the mutation induction of neutron radiation
beam used for BNCT in Kyoto University Research
Reactor (KUR).

No BPA

With BPANo BPA

With BPAHigh dose rate

Low dose rate

(20cG/min)( 4cG/min)

Neutron irradiation

Neutron irradiation

Fig.1 Induction of mutations in the HPRT locus in
CHO cells with or without BPA under the ascorbic
acid treatment. VC means Vitamin C which is anascorbate popular name.

MATERIALS & METHODS: The mutagenicity
measured by the frequency of mutations induced byneutron irradiation with or without boron compound.
The hypoxanthine-guanin-phosphoribosyl-transferase(HPRT) locus was examined in Chinese hamster ovary(CHO) cells irradiated with neutrons of KUR. A stock
solution of 10B-para-boronophenylanine (BPA) wasused for this experiment. Cell suspensions were incubated with BPA at 10 ppm concentration 1 hour before
neutron irradiation. High dose rate neutron irradiation
was 0.2Gy/min with 5MW of KUR, and low dose rate
neutron irradiation was 0.04Gy/min with 1MW of
KUR. Neutron fluencies were measured by radioactivation of gold foil and gamma-ray dose by TLD. After
neutron exposure, L-ascorbic acid was added to cells
at a final concentration of 5mmol/L and removed after
150 min of neutron irradiation. To determine mutation
frequencies, each treated culture was incubated with
non-selective medium for 7-9 days to allow phenotype
expression. Then, 2x105 cells were added to each dishcontaining 6-thioguanine and incubated for 10-14 days,
after which time the mutant colonies were counted.
The mutation frequency is expressed as the number ofresistant colonies divided by the total number of viable
cells as determined by cloning efficiency at the time of
selection.

0.2Gy/m in was 1.5-1.9 times and more increased thanat 0.04Gy/min in the function dose over the 1.8Gy.
These results suggested that dose rate effect is exist
neutron irradiation in BNCT. Ascorbic acid treatment
reduced mutation induction following neutron radiation. This protective effect of mutation induction was
more effective with BPA than without BPA. This resultshows that an ascorbate scavenged long-lived radicals
due to the nuclear capture reaction that of alpha particles or 7Li nuclei produced by 10B(n,) 7Li reaction,
not due to the reaction with normal tissue hydrogenand nitrogen. In neutron irradiation at high dose rate
(0.2Gy/min) with BPA, the mutation induction was
controlled most effectively. This result suggests thatthe ascorbate may protect the mutagenic effects of
BNCT on the normal tissue cells that take up the lowdose of boron compounds, for example the peri-tumoral stroma cells after BNCT.
In this study, we found that the ascorbic acid was
effective in protection of the mutation induction ofneutron radiation beam used for BNCT dose rate effectof the neutron radiation beam used for BNCT.
REFERENCES:[1] K. Kinashi et al., Appl. Radiat. Isot. , 88 (2014)
153-156.

RESULTS and DISCUSSION: Figure 1 shows themutation frequency in the HPRT locus in CHO cells
after neutron irradiation at 0.2Gy/min or at
0.04Gy/min with or without BPA. The frequency ofmutations after neutron irradiation with 10ppm BPA at

採択課題番号 26P3-1
BNC 反応により誘発される突然変異の解析（京大・原子炉）木梨友子、小野公二、高橋千太郎

㻝㻡

プロジェクトPR3-2Analysis of DNA Double Strand Breaks in the Mammalian Cells Induced by BNCR

S. Takahashi, Y. Kinashi, K. Seki, N. Yokomizo1, T.
Ikawa1, K. Ono, Y. Kubota2, and R. Okayasu2that difference of radiation sensitivity between A172 andT98G was decreased by BPA addition irradiation of neutron mixed beam.
These results indicate that the difference between theradiation sensitivity was observed between the T98G
cells and A172 cells boron neutron capture reaction. Interestingly, it was reduced with BPA where the irradiation
mainly depends on the particle radiation emitted by
BNCR (Boron Neutron Capture Reaction). This result
suggests that BNCT is an effective treatment withglioblastoma that can reduce the difference ofradiosensitivity by p53 functional status.

Research Reactor Institute of Kyoto University,
Graduate School of Agriculture, Kyoto University,
2
National Institute of Radiological Sciences
1

INTRODUCTION: Boron neutron capture therapy(BNCT) is a unique and effective treatment for cancer,
and now becoming a clinical application stage. However,
little is known about the biological effects of particle radiation induced by BNC reaction (BNCR) nor thermal-epithermal neutron beams for BNCT. In the present
study, we have investigated the most important biologicaleffects, i.e., DNA damages, after the irradiation withheavy ion particles from BNCR and neutron beam. In the
FY 2014, the relationship between the status of p53 andbiological effects (cell killing and induction of DNA
double strand breaks (DNA-dsb) was investigated.
EXPERIMENTS: Two types of human glioblastoma
cells, A172 and T98G were cultured. Both cells werepurchased from Riken BRC Cell Bank. A172 are wild
type of p53, and T98G cells are mutant type. The cells
were cultured in MEMα medium (Invitrogen) suppl
emented with 10% heat-inactivated FBS (Biowest) andmaintained at 37℃ in a humidified atmosphere with
5.0% CO2. The cells were irradiated at the KUR irradiation field for BNCT, with/without BPA. As a reference
radiation, Co-60 gamma-ray was used at the same dose
rate as the mixed irradiation. The cells were assayed forconventional colony formation, and DNA double strand
breaks (DSBs) were detected by immune-staining using
53BP1 antibodies.
RESULTS & DISCUSSION: The data on the cell survival are shown in Fig. 1 for the cell lines of A172 andT98G. In the case of not BPA added cells, A172 got thesteep slope graph of survival fraction. This shows T98G
cells have lower sensitivity to neutron mixed beam irradiation than A172. On the other hand, in the case of BPA
added cells, survival fraction curves of both cells weresimilar. This shows difference of radiation sensitivity
which confirmed the case of not added BPA cells declined by addition of BPA. When compared at 10% survival, in the case of not added BPA cells, A172 cells wererequired 1.663Gy radiation dose to cause 90% cell death,but T98G required 5.245Gy. This shows T98G were required the dose of 3 times more than the A172 to cause
90% cell death in the case of not added BPA, neutron
mixed beam irradiation alone cases. On the other hand, inthe case of added BPA cells, D10 of A172 indicated 0.821
Gy, and T98G indicated 1.076 Gy. This data indicatedFig. 1. Survival of glioblastoma cells (A172 andT98G) irradiated with thermal- to epithermal neutron
beam of KUR with/without BPA.
PUBLICATION:[1] K. Seki, Y. Kinashi, S. Takahashi:
The influence of p53 status in glioblastoma on the effects
of boron neutron capture therapy. Anticancer Research,
35: 169〜174, 2015.

課題採択番号 26P3-2 BNC 反応に伴う DNA 損傷、特に二重鎖切断とその修復の解析 プロジェクト（京大原子炉）高橋千太郎、木梨友子、関敬子、横溝夏弥、井川智之、小野公二（放医研）久保田善久、岡安隆一

㻝㻢

PR4

Project Research on Development of Scattering Spctrometers Utilizing Smalland Medium Class Neutron Source
ARS-4: Not performed by no operation of KUR.
ARS-5: Hara et.al. continued to analyze nanostructural change of a surfactant (Sodium Oleate, NaOl) with KUR-SANS. (The data was obtained in 2013). They analyzed the surfacta system with pair distance distribution function andrevealed spherical scatterers in the solution.
ARS-6: Not performed by no operation of KUR.
ARS-7: Not performed by no operation of KUR.
ARS-8: Not performed by no operation of KUR.

Masaaki Sugiyama
Research Reactor Institute, Kyoto University
Objectives and Allotted Research Subjects: It is no
doubt that Small-angle neutron scattering is one of themost powerful tools to investigate nanoscale structures invariety of materials. However, the less opportunity to do
SANS is a bottleneck that SANS becomes general method
to observe nanoscale structure. Utilizing small and medium size reactor as a neutron source for SANS spectrometer gives one answer for this difficulty. Under this line,
this project proves it through showing the feasibility andupgrade of KUR-SANS.
ARS-1: Challenge for Development of Analyzer for Particle-Size distribution with Small-Angle Scattering. (M.
Sugiyama, R.Inoue, N.Sato and Y. Oba)
ARS-2: Are Size Upgrading of Compact Monochromator for SANS. (M. Hino, Y. Oba, M.Sugiyama, T. Oda andS.Tasaki)ARS-3: Structural Analysis of PVA gel by adding Inorganic Salt (R.Inoue, Y. Oba, N. Sato, T.Kanaya and M.
Sugiyama)
ARS-4: Estimation of Fine Structure in Metallic Materials by SANS (Y. Oba, S.Morooka, M. Ohnuma, N. Sato,
M. Sugiyama)
ARS-5: KUR-SANS Observations and Analysis Surfactants’ Nano-structural Change by Capturing Heavy Metal.
(K. Hara, T. Miyazaki, Y. Oba, N. Sato, M. Sugiyama, Y.
Hidaka and H. Okabe,)
ARS-6: Small-Angle Neutron Scattering Analysis of the
Nanostructure of Wheat Proteins. (R. Urade, Y. Higashino,
S.Funaki, Y.Kitao, N. Sato and M. Sugiyama)
ARS-7: Structural Investigation on Radiation-Fabricated Functional Gel. (N. Sato, Y. Oba and M.
Sugiyama)
ARS-7: Quantitative Analysis for TiN particle byEffect of Thermal Weld in Steel (S. Morooka, Y. Oba,and M. Sugiyama)
ARS-8: Nano structure of metal hydride by neutron small
angle scattering. (K. Iwase, K. Mori, Y.Oba and M.
Sugiyama)
Main Results and Contents of This Project:

ARS-1: Not performed by no operation of KUR.
ARS-2: Not performed by no operation of KUR.
ARS-3: Not performed by no operation of KUR.

採択課題番号 26P4
中小型中性子源を用いた散乱分光システムの開発（京大・原子炉）杉山正明

17

プロジェクトPR4-1

KUR-SANS Observations and Analyses ofSurfactants’ Nano-structural Change by Capturing Heavy Metal

K. Hara, T. Miyazaki, Y. Oba1, N. Sato1, M. Sugiyama1,
Y. Hidaka, H. Okabe
Department of Applied Quantum Physics and Nuclear Engineering, Kyushu University
1
Division of Quantum Beam Material Science, Research Reactor Institute, Kyoto University
INTRODUCTION:
Ion flotation is well-known as a simple and useful
method to remove hazardous ions or to recover valuable ions [1,2]. Besides, because the surfactants are
known to exhibit various nano-scale structural changes in the flotation process as scavengers or collectors,
such a nano-structural change will be useful for examining the performance of KUR-SANS system installed at Research Reactor Institute, Kyoto University.
Therefore, in the present study, the nano-structuralchanges of a surfactant (Sodium Oleate, NaOl) in the
floatation process have been investigated.

Fig.1

SANS profiles of Sodium Oleatein D2O containing CuCl2 before flotation.

EXPERIMENTS:
CuCl2 (5 mM) was added to respective NaOl (30mM)-D2O solutions after adjusting their pHʼs at 7, 8, 10
and 12 with HCl and NaOH. Then the solutions were
bubbled for 10 min and were poured into quartz cells
for the SANS measurements. The SANS profiles were
measured at room temperature with the KUR-SANS
system (CN-2) with a 2.8 Å neutron beam.
RESULTS:
Figures 1 and 2 show SANS profiles of the CuCl2added Sodium Oleate in D2O at several pHʼsbefore andafter the flotation, respectively. Except for the pH=12
specimen, the lower-q region intensity decreased greatly indicating the larger substances are effectively recovered by flotation. In the present study, the SANS
profiles have been further analyzed with pair distance
distribution functions (PDDF) for deriving semi-quantitative scatterer-shape information [3]. As an example,
the PDDF of Cu-added pH=10 specimen is shown in
Fig. 3, of which the well-defined symmetric bell-shapeindicates the existence of spherical scatterers in the solution. Such features demonstrates a high quality of the
SANS profiles measured by the KUR-SANS system.

Fig.2

REFERENCE:[1] F. Sebba, Ion flotation (Elsevier, Amsterdam, 1962)[2] E. J. Mahne and T. A. Pinfold, J. Appl. Chem., 18(1968) 52-54[3] O. Glatter, J. Appl. Cryst., 10 (1977) 415-421

Fig.3

採択課題番号
ハイドロコロイドのガンマ線照射効果と(九大院工) 原 一広、宮崎智博
京大原子炉）佐藤信浩、大場洋次郎、杉山正明

18

SANS profiles of Sodium Oleatein D2O containing CuCl2 after flotation.

Pair distance distribution function of
Sodium Oleate in D2O containing CuCl2.

を用いたナノ構造観測 プロジェクト

PR5 Behavior of Radioactive Nuclides in Intense Radiation Fields in Accelerator Facilities
Y. Okitive aerosols in the target room of the KUR-LINAC. The
size and radioactivity of the aerosol sampled from two
sampling positions (40 cm and 230 cm apart from the Ta
target) were compared. The target was irradiated with the
30-MeV electron beams of 10, 50, and 100-µA currentsfor ~2 h per experiment. Radioactive aerosols were collected with a low-pressure cascade impactor to obtain theparticle size distribution. Under 10 µA and 50 µm, theparticle size distribution for radioactive aerosols showedno significant difference between the two sampling positions. Total radioactivity at both positions increased withbeam current.

Research Reactor Institute, Kyoto University
OBJECTIVES AND RESEARCH SUBJECTS:
High-energy and high-intensity accelerators are widelyused for many fields such as physics, chemistry and cancer therapy. The high-energy proton accelerators produce
a variety of radionuclides through nuclear reactions including spallation reactions in high-energy accelerator
facilities. The activation takes place in accelerator hardware, air, cooling water and other materials such as soil
outside of shielding concrete walls. From the viewpointsof radiation safety and safe accelerator operation, themanagement of the radionuclides is very important. The
behavior and property of the radionuclides are the mostimportant information to estimate radiation exposure andto ensure the accelerator safety.
In this work, the behavior and property were investigated in the air of the accelerator rooms and the coolingwater.
The following problems are studied in this work.
1. The property of radioactive airborne species (radioactive aerosols and radioactive gases) in the air.
2. The behavior of dissolved metals from cooling watertubes and radioactive nuclides formed in the water.
3. Problems related to activation in accelerator facilities
such as development of new radiation detectors forhigh energy accelerators and measurement of formation cross section of the principal radionuclides fordose estimation.

PRS-2
An air irradiation experiment was performed in the
150-MeV FFAG proton accelerator using an
air-irradiation chamber under various beam conditions.
The size and concentration of the aerosol particles produced in the irradiation were studied for applications to
the instrument calibration and other experiments using
standard aerosol particles. The size was increased as the
air supplying flow rate to the chamber was decreased. In
other words, the particles grew as the irradiation time wasincreased. The size was possible to be varied by changing
the flow rate to the chamber. In the case of 1 nA, beam
current, the size was able to be changed from approximately 10 to 20 nm in geometric mean diameter. The sizeand concentration were also dependent on the beam current. An increase in size and concentration was observed
above the proton current of approximately 300 pA andthey were almost saturated above 1 nA at the flow rate of
18 L/min

The participating research subjects (PRS) in the final
year of this project research (Fiscal 2014) and co-workers
in each subject are listed below.

PRS-3
In this work, experimental metal vessels filled withpure water were irradiated by -rays or bremsstrahlung /neutrons generated at electron linear accelerator (LINAC)
facility as model environments for cooling water used
inside accelerator facilities. Radiation effects on corrosion of various metals in water and colloid/particle formation of metal elements were systematically studied.
After the irradiation of -rays or bremsstrahlung, soluble(<3 nm), colloidal (3-200 nm), and particulate (>200 nm)
metal elements were detected in water. The size profiles
for each element in water and characteristics in radiation
effects were dependent on vessel materials. In the experiments using Al and Fe vessels, total Al/Fe concentrations became higher dependent on photon irradiation intensity. In the water supernatant obtained after the irradiations, Al and Fe were found to be mainly present as relatively-large particles (>200 nm). Concentrations of soluble species and fine colloidal species are quite small
compared to those of the large particle species. Theirchemical states were are also discussed in this work.

PRS-1 (26P5-1) Radioactivity Size Distribution of Airborne Aerosols Formed in Target Room Estimatedfrom Number Size Distribution(S. Yokoyama, Y. Oki and S. Sekimoto)PRS-2 (26P5-2) Production of Airborne Nano-Particles
by Proton Irradiation in an FFAG Accelerator(Y. Oki, N. Osada, S. Yokoyama, Y. Ishi, T. Uesugi, Y.
Kuriyama and M. Sakamoto)PRS-3 (26P5-3) Corrosion of Various Metals in Water
and Formation of Metal-related Colloidal Particles under Intense Photon-Radiation Field(K. Bessho, H. Matsumura, Y. Oki, S. Sekimoto, K.
Masumoto and N. Abe)
MAIN RESULTS:
PRS-1
The present study analyzed a distribution of radioac-

19PR5-1

Radioactivity Size Distribution of Airborne Aerosols
Formed in Target Room Estimated from Number Size Distribution

S. Yokoyama,1 Y. Oki,2 and S. Sekimoto2
1
2

rays induced by electrons.
Under 50 A, the peak radioactivity count collected at
port 2 was 1.3 times higher than that at port 1, as shownin Fig. 1. The number size distributions of aerosols simultaneously measured by a Scanning Mobility Particle
Sizer (TSI, Model 3080) showed a similar result. Radioactive aerosols are formed by deposition of radionuclides
on non-radioactive aerosols. Thus, the number of radioactive aerosols at port 2 under 50 A should increase. No
clear difference existed between median diameters ofradioactive size distributions at ports 1 and 2. This meansthat the non-radioactive aerosols were generated not onlyaround the target, but also throughout the target room.

School of Health Science, Fujita Health University
Graduate School of Engineering, Kyoto University

INTRODUCTION: To assess internal exposure of accelerator facility workers due to inhaling radioactive aerosols and gases, the radioactivity size distribution and theamount of radioactive aerosols formed in the facilities
must be estimated [1–4]. In previous studies, aerosol radioactivity and number size distributions were measured
in the target room of KUR-LINAC and the radioactivity
size distributions were estimated from the number-size
distributions [3, 4]. In addition, the relationship between
radioactivity size distribution of aerosols and beam currents was investigated. The present study analyzes a distribution of radioactive aerosols in a target room.

15000

dA/dlogDp

EXPERIMENTS: Two sampling ports were prepared 40
cm (port 1) and 230 cm (port 2, near the wall surface)from the target of KUR-LINAC. Electron beams weregenerated under a 30-MeV voltage and 10-, 50-, and100-μA currents for ~2 h per experiment. A water-cooled
Ta target was placed at the end of the beam line as a neutron generator. Radioactive aerosols were collected by a
13-stage low-pressure cascade impactor (Tokyo Dylec
Corp.). Stainless steel plates coated with grease were set
in each stage, except for the lowest stage, in which a filter
was set. The collection started at 60 min after irradiation
began and continued for 30 min. After collection, theplate and filter radioactivities were measured by a GM
survey meter (TGS123-C, Aloka). Radionuclides formedin the target room confirmed that 13N contributed significantly to total activity, when compared with the lower
radioactivity measured in the previous study [4].
RESULTS: Figure 1 shows the radioactivity size distribution of aerosols under 10- and 50-A beam currents at
ports 1 and 2. Under 10 A, the median diameters of radioactive aerosols were 270 and 189 nm (and 1.2)
at ports 1 and 2, respectively. Under 50 A, median diameters of radioactive aerosols were 270 and 229 nm(and 1.4) at ports 1 and 2, respectively. In the previous study, the median diameter of radioactive aerosols
collected near the target was 261±3.9 nm under 20-100
A [3, 4]. Figure 2 illustrates the total radioactivity ofaerosols under 10, 50 and 100 A. Total radioactivity at
ports 1 and 2 increased with beam current.
Radionuclides are mainly generated by interaction between neutrons and the atmospheric nitrogen and oxygen
proximal to the target just after the electron beam hits thetarget. Non-radioactive aerosols were formed by irradiation by electrons leaked from the beam line and gamma

10A, at 40 cm
10A, at 230 cm
50A, at 40 cm
50A, at 230 cm

10000

5000

0

100

1000

10000

Diameter (nm)F
ig. 1. Activity size distribution of radioactive aerosols
collected at ports 1 and 2.

Total activity (Counts)

60000
50000
40000
30000
20000

at 40 cm
at 230 cm

10000
0

0

20

40

60

80

100

Beam current (A)

Fig. 2. Total activity of radioactive aerosols at ports 1 and
2.
REFERENCES:[1] S. YOKOYAMA et al., Jpn. J. Health. Phys., 43(2008) 333–340.
[2] S. YOKOYAMA et al., Rad. Prot. Dosi., 127 (2007)
392–397.
[3] S. YOKOYAMA et al., KURRI progress report 2012,
PR11-1 (2013), http://www.rri.kyoto-u.ac.jp/JRS/.
[4] S. YOKOYAMA et al., KURRI progress report 2013,
http://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep201
3/Project8.pdf

採択課題番号 26P5-1
加速器施設内生成粒子の粒径分布に関する研究（藤田保衛大・医科）横山 須美（京大・原子炉）沖 雄一、関本 俊

20

プロジェクトPR5-2 Production of Airborne Nano-Particles by Proton Irradiation in an FFAG Accelerator
Y. Oki, N. Osada1, S. Yokoyama2, Y. Ishi, T. Uesugi, Y.
Kuriyama and M. Sakamoto

the beam dump of the specimen irradiation beam line.
The 1-mm thick aluminum plates were used as both endsof the chamber. The aerosol-free air was prepared by filtration and was introduced to the chamber at the constantflow rate, and the irradiated air was sampled from thechamber at the same flow rate.
The size distribution and the total concentration of theaerosol particles were measured with SMPS (Scanning
Mobility Particle Sizer).

Research Reactor Institute, Kyoto University
Advanced Science Research Center, Okayama University
2
School of Health Science, Fujita Health University
1

INTRODUCTION: In accelerator facilities, very fineradiation-induced aerosol particles were often producedin air of accelerator rooms during machine operation. The
size and concentration of the particles are generally very
stable under a given beam condition. This particle generation may be applicable to calibration of size-measuring
instrument for the fine particles in the diameter range ofnm to 0.1 m.
In this work, an air irradiation experiment was performed in an FFAG (Fixed Field Alternating Gradient)
proton accelerator under various beam conditions. The
size and concentration of the aerosol particles producedin the irradiation were studied for applications to the instrument calibration and other experiments using standard aerosol particles.

RESULTS AND DISCUSSION: The size of formed
aerosol particles showed very steady mono-modal
log-normal distributions. The size was increased as the
air supplying flow rate was decreased. In other words,
the particles grew as the irradiation time was increased.
The size was possible to be varied by changing the flowrate to the chamber. In the case of 1 nA, beam current,
the size was able to be changed from approximately 10
nm (the flow rate: 18 L/min) to 20 nm (8 L/min) in geometric mean diameter. The size and concentration werealso dependent on the beam current. An increase in sizeand concentration was observed above the proton currentof approximately 300 pA and they were almost saturated
above 1 nA at the flow rate of 18 L/min [1].
During the air irradiation, principal radionuclides
formed in the accelerator air, 15O (half life: 2 min), 13N(10 min), 11C (20 min) [2] and 7Be (53 d), are formed
together with the radiation-induced aerosol particles. The
aerosol particles form radioactive aerosols by incorporating the radioactive atoms into the radiation-induced particles. The size distribution of 7Be-bearing aerosol particles were successfully measured with a graded screen
array system in the same air-irradiation chamber [1]. The
7
Be aerosol particles can be also used in various research
including calibration of aerosol instruments for radioactive fine particles.

EXPERIMENTS: The irradiation experiment was performed in the 150-MeV FFAG proton accelerator of Research Reactor Institute, Kyoto University (KURRI). The
FFAG accelerator system consists of the 11-MeV H– linear accelerator (Injector) and the FFAG main ring. The
injected protons are accelerated in the main ring to 150
MeV after conversion of H– ions to protons. The nominal
150-MeV proton beams were extracted to an air irradiation chamber in the specimen irradiation beam line. Figure 1 shows the irradiation chamber together with thespecimen irradiation beam line and the main ring.

In conclusion, the air-irradiation chamber was capable of producing aerosol particles in the diameter rangeof 10 to 20 nm by the 1-nA proton irradiation carried out
in the FFAG accelerator.
REFERENCES:[1] Y. Oki, N. Osada, Y. Ishi, T. Uesugi, Y. Kuriyama and
M. Sakamoto, KEK Proceedings 2014-7, 52-57.
[2] A. Endo, Y. Oki, Y. Kanda, T. Oishi, and K. Kondo,
Radiat. Prot. Dosim., 93 (2001) 223-230.

Fig.1 Irradiation Chamber
The air-irradiation chamber was a 1-m long stainlesssteel cylinder (i.d. 15 cm). It was installed upstream of

加速器室の空気生成する放射性化学種の生成挙動
採択課題番号 26P5-2（京大・原子炉）沖 雄一、関本俊、（藤田保健衛生大医療科学部）横山須美
21

プロジェクトPR5-3

Corrosion of Various Metals in Water and Formation of Metal-related
Colloidal Particles under Intense Photon-Raiation Field

K. Bessho, H. Matsumura, Y. Oki1, S. Sekimoto1,
K. Masumoto, N. Abe1

alloys). In this report, some characteristics observed forpure Al, Fe and Cu are described.
In the experiments using Al and Fe vessels, irradiations
were carried out at LINAC with two kinds of beam currents (20, 100 A) and the irradiation times of 2 h. Total
Al/Fe concentrations became higher dependent on photon
irradiation intensity. In the water supernatant obtained
after the irradiations, Al and Fe were found to be mainlypresent as relatively-large particles (>200 nm). Concentrations of soluble species and fine colloidal species arequite small compared to those of the large particle species.
Al and Fe in non-degassed water are considered to be in
the oxidation states of III (Al3+, Fe3+), which tend to formhydroxide precipitations in neutral pH conditions. It canbe supposed that photon irradiation facilitates the corrosion (oxidation) of pure Al and Fe metals in water, consequently Al and Fe are released as Al3+, Fe3+ ions fromthe metal surface to water, finally form Al(OH)3 andFe(OH)3 particles in water phase.
In case of the experiments using Cu metal vessels, effects of radiation were mainly observed as increase insoluble Cu species (<3 nm) and production of large particle Cu species (>200 nm). Under irradiation conditions,soluble Cu concentration increased with time depend on
photon doses and finally reached to plateau, which may
be originated from hydrolysis of Cu(II) ions. On the other
hand, production of particle Cu species was observed
remarkably after long irradiation times (> 20-30 h). These
characteristic time-dependence imply that particle Cu
species were initially generated at the Cu/water interface
as particle-like corrosion products. These products grewup at the interface in a time scale of several tens hours,
and were finally released into water phase as particles (>200 nm). The particle production processes at the interface were also promoted by photon irradiations [3].
Radiation effects on corrosions of metals in water are
explained by production of oxidative reactive species,
such as OH radicals and H2O2, induced by radiolysis ofwater molecules. By using water quality testing kits, it
was demonstrated that several mg/L of H2O2 and O3 were
produced by irradiation of water by -rays or bremsstrahlung, and these oxidative species should induce various radiation effects clarified by this work.

Radiation Science Center, KEK
1
Research Reactor Institute, Kyoto University
INTRODUCTION: At high-energy accelerator facilities, intense radiations affect chemical states of elements
including radionuclides inside the facilities. In the cooling-waters for various accelerator components, corrosionof metal components and formation of metal related colloids/particles in water are important subjects in the radiation safety managements at accelerator facilities, because some radionuclides are incorporated in colloidal
species and it complicate the behavior of nuclides [1,2].
In this work, experimental metal vessels filled withpure water were irradiated by -rays or bremsstrahlung /neutrons generated at electron linear accelerator (LINAC)
facility as model environments for cooling water used
inside accelerator facilities. Radiation effects on corrosion of various metals in water and colloid/particle formation of metal elements were systematically studied.
EXPERIMENTS: Metal vessels (I. D. 19 x 75 mm)
filled with pure water were irradiated by -rays generated
at the 60Co -ray irradiation facility, or bremsstrahlung /neutrons generated by 30 MeV electron beam hitting on a
Ta target (50 x 62 mm) at the LINAC facility. Samples
at the LINAC experiments were placed at the downstream position (40 or 80 mm from Ta target) and perpendicular position (40 or 80 mm from Ta target).
Monte Carlo calculations and activation experiments using metal foils (Au, Al) demonstrated that radiation effects observed in the present LINAC experiments could
be ascribed to the effects of photon irradiations (maximum fluxes; 3 MeV for 0-deg and 0.7 MeV for 90-deg).
Contribution of neutrons was found to be much smaller
than those of photons in these experiments.
After the irradiations, water in metal vessels werepoured out and treated with four kinds of ultrafiltration(UF) membrane units for particle size separation contained in water supernatant. Estimated pore sizes of the
UF units were 200, 16, 7 and 3 nm. Concentrations ofmetal elements in the filtrates and unfiltered samples
were determined by ICP-AES analyses.

REFERENCES:[1] K. Bessho et al., J. Radioanal. Nucl. Chem., 303(2015) 1719-1725.
[2] H. Matsumura et al., Progress in Nucl. Sci. Technol.,
4 (2014) 372-375.
[3] K. Bessho et al., J. Radioanal. Nucl. Chem., 303(2015) 1117-1121.

RESULTS: After the irradiation of -rays or bremsstrahlung, soluble (<3 nm), colloidal (3-200nm), andparticluate (>200nm) metal elements were detected inwater. The size profiles for each elements in water andcharacteristics in radiation effects were dependent on
vessel materials (pure Fe, Al, Cu, and SUS-304, A6061

採択課題番号 26P5-3

高線量放射線場における水中金属材料の腐食およびプロジェクトコロイド生成挙動の解析２（KEK・放射線）別所光太郎、松村宏、桝本和義（京大・原子炉）沖雄一、関本俊
22

PR6

Irradiation Effects on Nuclear Advaced Materials Irradiatedby Particles with High Energy
Electron irradiation on W at around 500 ℃ using
KURRI-LINAC(M. Akiyoshi, T. Yoshiie, Q. Xu and K. Sato)
ARS-6
The development of new positron beam system using
KUR(Y. Nagai, K. Inoue, T. Toyama, Y. Shimizu, K. Nagumo,
M. Shimodaira, T. Hirota, K. Sato, T. Yoshiie and Q. Xu)
ARS-7
Radiation damage in bulk amorphous alloys by electron
irradiation(F. Hori, K. Ishii, T. Ishiyama, K. Kobayashi, A. Iwase, Y.
Yokoyama, Q. Xu and K. Sato)
ARS-10
Positron annihilation study of Fe-Cr alloys after neutron
irradiation in KUR(R. Kasada, K. Sato and Q. Xu)
ARS-12
Positron annihilation lifetime measurements austenitic
stainless steels irradiated in the SINQ target irradiation
program(K. Sato, Q. Xu, T. Yoshiie, Y. Dai and K. Kikuchi)
ARS-13
Effects of high energy particle irradiation on hydrogen
retention in refractory metals(K. Tokunaga, M. Matsuyama, S. Abe, H. Osaki, K. Araki, T. Fujiwara, M. Hasegawa, K. Nakamura, Q. Xu and
K. Sato)ARS-14
Dependence of cellular structure formation on ion species(N. Nitta, C. Watanabe, M. Taniwaki, Q. Xu and T.
Yoshiie)Q. Xu
Research Reactor Institute, Kyoto University
OBJECTIVES: Neutron irradiation is usually used toinvestigate radiation effects in solid materials and develop new materials. Unfortunately, because the operation
time of KUR was limit, and the laboratory for neutron-irradiated samples could not be used in 2014, theresearch activities were severely restricted. In the present
report, instead of neutron irradiation, ion, electron and γ
ray irradiations were used to estimate degradation mechanical properties of materials, such as material for optoelectronic and high-power devices.
RESULTS: The allotted research subject (ARS) andthe name of co-researches in each ARS are listed below.
ARS-1
Compensation mechanism of DX-like center in neutrontransmutation doped GaN(K. Kuriyama, T. Nakamura, A. Shikawa, K. Kushida,
and Q. Xu)
ARS-2
Neutron irradiation effects of superconducting magnet
materials at low temperature(T. Nakamoto, M. Yoshida, T. Ogitsu, Y. Makida, K. Sasaki, S. Mihara, K. Yoshimura, H. Nishiguchi, M. Sugano,
M. Iio, Y. Yang, Y. Kuno, M. Aoki, A. Sato, Q. Xu, K.
Sato, Y. Kuriyama and Y. Mori)
Candidate materials, such as Al and Cu alloys, for superconducting magnets of upgraded LHC at CERN andthe muon source for the COMET experiment at J-PARC
were irradiated by LTL at ~10 K. In Al alloys, almost
100% of the defects produced by the irradiation was recovered after warming up to room temperature, however,
several percent of the defects was remained in Cu alloyeven at room temperature.
ARS-3
Study on fine structures formed by high energy particle
irradiation(A. Kinomura, K. Sato, Q. Xu and T. Yoshiie)
ARS-4
Thermoluminescence of Synthesized Calcite(T. Awata, K. Nakashima and Q. Xu)
ARS-5

採択課題番号 26P6

CONCLUSIONS: The defects induced by irradiation
degrade the physical mechanical properties of solid materials. Part of the physical and mechanical properties canbe recovered at high temperatures where defects are mobile. Some experimental results are important for development of large equipment. For example, the results of
ARS-2 indicate that Al alloys can be used in high energy,
high-power accelerator as the material of superconducting magnets since the defects produced by the irradiation
recover when the magnets are warmed up to room temperature.

原子力先進材料における高エネルギー粒子線の照射効果（京大・原子炉）徐 虬

23

プロジェクトPR6-1 Compensation Mechanism of DX-like Center in Neutron Transmutation Doped GaN
K. Kuriyama, T. Nakamura, A. Shinkawa, K. Kushida1,
and Q. Xu2

n = 2(mekBT/2πħ2)3/2exp[(EF-Eg)/kBT],

College of Engineering and Research Center of Ion
Beam Technology, Hosei University
1
Osaka Kyoiku University
2
Research Reactor Institute, Kyoto University

where me is the effective mass of GaN, kB the Boltzmann’s constant. Therefore, the increase of the carrier
concentration with increasing the temperature would be
attributed to the thermal excitation to the conduction bandof electrons trapped in Ni acceptors, as shown in Fig. 1(b).

INTRODUCTION: The 1000 ºϹ annealed neutrontransmutation doped (NTD)-GaN keeps having high resistivity of 108 Ωcm at room temperature. In the present
study, we report the compensation mechanism of DX-likecenter of the neutron transmuted Ge in NTD-GaN.
EXPERIMENTS: GaN epitaxial films on sapphire substrates were irradiated with fast and thermal neutrons atfluences of 6.7 x 1018 cm-2 and 1.4 x 1019 cm-2, respectively. We carried out an alternating current (ac)-Hall
effect measurement and clarified the existence of deepenergy level from the temperature dependence of carrier
concentration in high temperature region.
RESULTS: The resistivity and carrier concentration of
the 1000 ºϹ annealed samples were 2.47 x 106 Ωcm,
4.13 x 1010 cm-3 at 150 ºϹ and 2.37 x 103 Ωcm, 1.60 x1014 cm-3 at 400 ºϹ, respectively. All annealed samples
showed the n-type conduction. The carrier concentration
at both 150 ºϹ and 400 ºϹ were much lower than thecalculated transmuted-Ge concentration (1.24 x 1018cm-3). Fig. 1 (a) and (b) show the schematic diagram of
impurity levels of NTD-GaN. Ge atoms transmuted in
GaN by the two (n,γ) reactions of 69Ga and 71Ga form theDX-like center as donor [1]. Ge is localized at 500 meV
below the bottom of the conduction band from results ofphotoluminescence (PL) measurements [1], supporting
the results of the theoretical calculation [2]. N interstitial(Ni ) atoms generated by NTD-process form the deep
acceptor level at 960 meV below the bottom of the conduction band from present study.14C atoms generated bythe (n,p) reaction are substituted to N sites and forms theacceptor level at 230 meV above the top of the valenceband [3], consistent with the result from the PL measurements[4]. Since the carrier concentration of
NTD-GaN cannot be measured at room temperature,DX-like center of Ge is compensated by both 14C and Ni
acceptors. The Fermi level estimated from the following
equation [5] for a temperature range of 150 - 400 ºϹ was
650 ± 25 meV.

Fig 1. The schematic diagram of impurity levels in
NTD-GaN. (a) the compensation of DX-like center of Ge
donors by 14C and Ni acceptors. (b) the thermal excitationfrom the energy level of N interstitial.
A part of KURRI Progress Report has been publishedin Solid State Communications, 205, 1 (2015).
REFERENCES:[1] K. Kuriyama, T. Tokumasu, Jun Takahashi, H. Kondo,
and M. Okada, Appl. Phys. Lett. 80, 3328 (2002);
Proccedings of 26th Int. Conf. Physics of Semiconductors (Edinburgh, UK) D46 (2002).
[2] P. Boguslawski, J. Bernholc, Phys. Rev. B 56, 9496
(1997).
[3] J. Neugehauer, C. G. Van de Walle, Phys. Rev. B 50,
8067 (1994).
[4] T. Ida, T. Oga, K. Kuriyama, K. Kushida, Q. Xu, andS. Fukutani, AIP Conference Proceedings, 1566, 67(2013) (31st Int. Conf. Physics of Semiconductors,
Zurich, Switzerland, 2012).
[5] G. Burns, in Solid State Physics, (Academic Press, Inc,
1985) Chap.2.

採択課題番号 26P6-1 化合物半導体の照射効果と電気的・光学的物性に関する研究（法政大院）栗山一男、中村 司、新川 輝、（大阪教育大）串田一雅（京大・原子炉）徐 虬
24

プロジェクトPR6-2

Neutron Irradiation Effects of Superconducting Magnet
Materials at Low Temperature

T. Nakamoto, M. Yoshida, T. Ogitsu, Y. Makida, K. Sasaki, S. Mihara, K. Yoshimura, H. Nishiguchi,
M. Sugano, M. Iio, Y. Yang1, Y. Kuno2, M. Aoki2,
A. Sato2, Q. Xu3, K. Sato3, Y. Kuriyama3, and Y. Mori32011 - 2013, CX-1070-SD for 2013 - 2014) showed atemperature drift during neutron exposure due to theirradiation damage. The thermocouple and the Cernox
sensor were placed just behind the samples to measure
the temperature of the helium gas coolant.

J-PARC Center, KEK
1
Department of Applied Quantum Physics & Nuclear
Engineering, Kyushu University
2
Department of Physics, Osaka University
3
Research Reactor Institute, Kyoto University

RESULTS: The fourth irradiation test for the aluminum sample (Al-Y2) and the copper sample was carriedout in April 2014. Another type of aluminum sample with
Ni additive (Al-Ni) was also irradiated at second time.
The irradiation condition is basically same as the previous irradiations. After cooling down to 12 K, the reactor
was turned on to a power of 1 MW. The estimated fastneutron fluence in 53.5 hours operation is 2.7 x 1020 n/m2.
Behavior of the induced resistance by the neutron irradiation is very similar to the previous results. Degradation
rates of the electrical resistivity for both aluminum samples
are
quite
similar:
2.2 x 10-31 "m3
and
-31
3
2.3 x 10 "m for Al-Y2 and Al-Ni, respectively. For
copper sample, the degradation rate is 7.3 x 10-31 "m.
After the irradiation, all samples were warmed up to
room temperature. Anneal effects of the samples were
measured at the subsequent cooling test to 12 K in December 2014 without irradiation. Table 1 lists the summary of irradiation tests so far. For the aluminum samples, the induced resistance was fully recovered to be theoriginal resistance for all cases while the degradation rate
is much higher than copper. This means that the degradedelectrical resistivity of aluminum stabilizer in the superconducting magnet due to the irradiation can be completely recovered by the adequate intervention of warming up to room temperature. For the copper sample,
however, the recovery of the resistance by the thermal
cycle was imperfect for all cases: the recovery rates were
82 % to 96 %. This will concern the safe operation of thesuperconducting magnet at severe radiation environment.

INTRODUCTION: Superconducting magnets will be
subjected to a high neutron fluence of 1021 n/m2 or higher
in the operation lifetime in the high energy particle physics experiments, such as a high luminosity upgrade of the
LHC at CERN and the muon source for the COMET experiment at J-PARC. Since electrical resistivity of a stabilizer at low temperature, which is very sensitive to neutron irradiation, is one of the important parameters for thequench protection of the magnet system. A series of electrical resistivity measurement at neutron irradiation for
the aluminum stabilizer with additives of yttrium takenfrom the prototype superconducting cable as well as
copper stabilizer was started in 2011. In 2014, the fourth
irradiation test with the same samples which were irradiated so far was performed to observe the effect of themultiple irradiations and the thermal cycles to room temperature on the electrical resistivity.
EXPERIMENTS: The irradiation tests have been carried out at a low temperature irradiation facility (LTL) at
E-4 line of KUR. Detailed experimental procedure wasreported in [1]. The aluminum stabilizer samples withdimensions of 1 mm x 1 mm x 70 mm were cut from thesuperconducting cable manufactured by Hitachi Cable.
The copper stabilizer sample has the dimensions of!1mm x 50mm. The electric resistance was measured by
a 4-wire method employing a Keithley 6221 current
source and a Keithley 2182A voltmeter. The temperature
was determined by using a thermocouple of Au(Fe) and
Chromel, since the Cernox sensor (CX-1050-SD for

REFERENCES:[1] M. Yoshida et al., Proc. of ICEC 24-ICMC 2012,685-688, 2013.

Table 1. Summary of irradiation effects on electrical resistivity of stabilizers with multiple neutron irradiations.
Sample, irradiation year
2011
2012
Al-Y2
2013
2014
2013
Al-Ni
2014
2011
2012
Copper
2013
2014

Initial RRR
360
360
368
367
561
566
308
291
285
277

Tirr (K)
12
15
15
14
15
14
12
15
15
14

#tot (>0.1 MeV) (n/m2)
2.6 x 1020
2.6 x 1020
2.6 x 1020
2.7 x 1020
2.6 x 1020
2.7 x 1020
2.6 x 1020
2.6 x 1020
2.6 x 1020
2.7 x 1020$%irr/#tot x10-31 ("m3)
2.8
2.9
2.5
2.2
2.6
2.7
0.93
1.02
0.77
0.73

Recovery Rate (%)
100
100
100
100
100
100
82
92
95
96

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25

PR6-3

Study on Fine Structures Formed by High Energy Particle Irradiation

A. Kinomura*, K. Sato1, Q. Xu1 and T. Yoshiie1

triangle), where the room temperature was assumed to be
27 °C.
Types of major annealed defects are different
depending on the irradiation temperature in the current
temperature range (from room temperature to 400 °C).
Damage peak after thermal annealing at 400 °C was close
to the undamaged level in the RBS/C spectrum, whereas
the damage peak after thermal annealing at 90 °C (in thisstudy) was close to the random level. In spite of thedifference in annealed defects, the Arrhenius plot
provides some insights in terms of the comparison
between neutron-enhanced and ion-beam annealing.
The difference in efficiency between neutron-enhanced
and ion-beam annealing was within one order ofmagnitude, implying that a similar mechanism may be atwork for both of annealing methods.
In summary, the effect of neutron irradiation on
ion-implantation induced damage in Si was investigatedusing the neutron irradiation in KUR. Similar annealing
efficiencies were obtained for neutron-enhanced andion-beam annealing experiments.
ACKNOWLEDGMENT: We would like to thank K.
Yasuda and R. Ishigami of the Wakasa Wan Energy
Research Center and colleagues of AIST for theirassistance on this study.
REFERENCES:[1] A. Kinomura, T. Yoshiie, A. Chayahara, Y. Mokuno,
N. Tsubouchi, Y. Horino, Q. Xu, K. Sato, K. Yasuda, and
R. Ishigami, Nucl. Instrum. Methods Phys. Res. B 334(2014) 48.
[2] A. Kinomura, A. Chayahara, Y. Mokuno, N.
Tsubouchi, Y. Horino, T. Yoshiie, Y. Hayashi, Q. Xu, Y.
Ito, R. Ishigami and K. Yasuda, Appl. Phys. Lett. 88(2006) 241921.

National Institute of Advanced Industrial Science andTechnology (AIST)
1
Research Reactor Institute, Kyoto University*Present address: Research Reactor Institute, Kyoto
University
INTRODUCTION: The effects of ion irradiation havebeen extensively studied for various crystalline materials.
It is known that irradiation causes the damage ofcrystallinity, leading to the degradation of original
material properties.
However, under particular
irradiation conditions, the irradiation effects can induceinteresting phenomena such as ion beam annealing in Si,
where crystallinity of implantation-induced damage
layers are recovered by other ion irradiation. Thus, it isimportant to investigate the irradiation effects ofenergetic particles (ions and neutrons) and the influenceon crystallinity of materials.
EXPERIMENTS:
Neutronenhancedannealing(crystalline recovery) of ion-implantation induced
damage in single-crystalline Si has been investigated tocompare the difference in annealing effects between ion
and neutron irradiations.
Si ion implantation to(100)-oriented Si was performed at 200 keV to a dose of
5×1014 cm-2 to introduce irradiation damage in the sample.
The Si-implanted sample was encapsulated in an Al
capsule with He ambient gas and neutron irradiated for
12 weeks in the core irradiation facility of the Kyoto
University Reactor (KUR) operating at 5 MW. Control
samples were thermally annealed at 90 °C in a quartz
tube furnace with flowing Ar gas for the same annealing
time as the neutron irradiation. The damage levels ofsamples were measured by Rutherford backscatteringwith channeling (RBS/C) using a 2 MeV He ion beam.
RESULTS: Sample temperatures cannot be directly
measured during reactor operation in the case of the KUR
core irradiation facility. In this study, the sample
temperature during the neutron irradiation was estimatedto be below 90 °C by solving a partial differential
equation describing the heat flow inside the sample
capsule made of Al. Since the thermal annealing rate
for heavily damaged Si was nearly constant around 90 °C,
the error of estimated temperature rise does not affect theresult of this irradiation experiment.
The samples before and after irradiation were
measured and damage levels were calculated by taking
account of dechanneling fractions in RBS/C spectra.
Annealing efficiencies obtained in this and previous
studies [1, 2] were plotted (closed circles), under theassumption that the irradiation temperature in this study
was 90 °C. For comparison, efficiencies of ion beamannealing of disorder were also calculated from the databy other groups and plotted in Fig. 4 (closed square andFig. 1 Annealing efficiencies of neutron and ion-beamirradiations.
Closed circles (neutron), triangle andsquare (ion) correspond to the original efficiencies.
Open circles (neutron), triangle and squares (ion)correspond to the efficiencies corrected based on
displacement-rate dependence.

採択課題番号 26P6-3 高エネルギー粒子照射に関わる材料の微細構造の研究（産総研）木野村淳 （京大・原子炉）佐藤紘一、徐
、義家敏正
26

プロジェクトPR6-4

Thermoluminescence of Synthesized Calcite

T. Awata, K. Iwasaki, S. Tanaka, Q. Xu1

X-, Y- and Z- axes indicate emission wavelength (nm) of
emission, temperature and intensity, respectively. Thereis one peak at 620nm starting from 285K same result as

Department of Physics, Naruto University of Education
1
Research Reactor Institute, Kyoto University
INTRODUCTION: We reported that thermoluminescence (TL) of natural calcite (CaCO3) irradiated by
gamma rays [1-2]. In that result, it was shown that thealmost spectra of TL had only one orange emission peakat 620nm, and that may be originated from a small
amount of impurity of Mn2+ in Calcite [3]. In this study,
we have artificially synthesized calcite with different
kinds of impurity using chemical reaction in water solution, and compared TL spectra of these with natural calcite, and to clear the relationship with emission and kindsof impurity.

Fig. 2 TL 3D spectrum of synthesized calcite with Mn
irradiated by gamma rays.
former our experiment of natural calcite [2]. It is clearthat 620nm emission peak at calcite is originating fromexistence of small amount of Mn. This result is supported
by study of Medlin [3]. Figure 3 shows those TL spectraof synthesized calcite with Mn, Mn+Ce and Mn+Pb at
maximum intensity temperature. Mn and Mn+Pb spectra
looks alike, and have one peak at 620nm same as former
our experiment. As Mn+Ce spectra, it has one peak at
640nm which is different from other two samples. Comparing this result with photoluminescence one makes it
possible to be clear that reason.

EXPERIMENTS: Calcites were synthesized by achemical reaction method in water solution [4]. 1.5% of(NH4)2CO3･H2O(1.5g in 100mL pure water) and 1.8% of
CaCl2･6H2O (2g in 100mL pure water) with 0.01g element impurity were mixed at room temperature. After
mixed, these solutions were precipitated by holding for
two weeks, and filtering. After filtering, samples wereshaped by a tablet machine. We have made three samples
with different element impurities (Mn, Mn+Ce, Mn+Pb).
These samples were irradiated 60Co gamma rays for 1h(about 20kGy) at 77K using KUR gamma-ray facility.
The thermoluminescence spectra were measured by aphoto-spectrometer (Princeton Instrument Spectra Pro
300i) with a temperature controlled system (77K to413K).

4[ 10 ] 5

Intensity (arb.)

4

RESULTS and DISCUSSION: Fi gur e 1 s ho ws t hethermoluminescence picture of synthesized calcite with
an impurity Mn and Mn+Ce by gamma rays irradiation.
This picture was taken by stereo microscope after pick-

Mn
Mn+Ce
Mn+Pb

3
2
1
0

400

500

600
700
wave length (nm)800

Fig.3 TL spectra of synthesized calcite with Mn,
Mn+Ce and Mn+Pb.
REFERENCES:[1] T. Awata, T. Kishino, F. Maki and Q. Xu, KURRI
Progress Report 2011, p.143.
[2] T. Awata, K. Nakashima and Q. Xu, KURRI Progress
Report 2013 p.169.
[3] W. L. Medlin, J. Opt. Soc. Am. 53(1963)1276.
[4] G. R. Fonda, J. Phys. Chem. 44(1940)435.

Fig. 1 Thermoluminescence of synthesized calcite with
an impurity of Mn (left) and Mn+Ce (right).
ing out from liquid nitrogen. Both pictures show orange
emission almost same as natural calcite with Mn element[2]. Figure 2 shows a 3D thermoluminescence spectrumof calcite with Mn impurity irradiated by rays at 77K
from 93K to 413K with heating speed at 0.32K/second.

採択課題番号 26P6-4
イオン性結晶材料の放射線誘起発光機構（鳴門教育大学）粟田高明、岩崎健太郎、 田中聡（京大・原子炉）徐虬
27

プロジェクトPR6-5

Electron irradiation on W around 500℃ using KURRI-LINAC

M. Akiyoshi1, T. Yoshiie2, Q. Xu2, K. Sato2

nuclear reaction will activate Ag atoms very strongly, so
it cannot be used. In addition, conventional (horizontal)
graphite sheet (Panasonic PGS graphite sheet,
EYGS-182310 t=0.10mm, TC=700W/m・K) is used tospread heat horizontally.
The piled graphite sheets and specimen holders aretighten with screws and nuts made by Ti to avoid radio
activation. This pile is put between Al square tubes withthe vertical-graphite seats. All specimens and Cu plates
are coated by BN spray to avoid surficial oxidation. In
addition, a Cu aperture was put in front of the specimen
pile to trim down the beam irradiated on out side of thespecimen that heats the pile wastefully.
Pure W specimens (Nilaco) was cut into φ10 and thethickness was 0.5mm (2 pieces) and 1.0mm (1 peace). α-Al2O3, β-SiC specimens （φ10×0.5mm）are also
irradiated.

1

Faculty of Engineering, Kyoto University(from 2015.04: Radiation Research Center, Osaka Prefecture University )2
Research Reactor Institute, Kyoto University
INTRODUCTION:
It is well known that irradiation induced damages inceramics showed significant degradation in thermal diffusivity unlike metals. In addition, the dependence ofthermal diffusivity on measurement temperature is affected with irradiation induced damages. Therefore,
thermal diffusivity during the irradiation is still not estimated. To resolve this problem, kinetic analysis is required where most important information is the behaviorof point defects. Electron irradiation is the best choice toinduce simple Frenkel pairs.
In these days, W (tungsten) material is considered as a
candidate for divertor material in future fusion reactor. W
is metal, of cause, but showed a similar behavior ofthermal diffusivity. It shows relatively small thermal diffusivity arisen from low electron conductivity, but shows
dependence on measurement temperature like ceramics
caused by phonon-phonon scattering.
In this study, we irradiated W specimen using KURRI-LINAC and check the specimen temperature during
the irradiation, and also radio-activity of specimens.

RESULTS:The beam condition was Acc. Energy: 32MeV, Pulse
length 4s, Peak current: 550mA. The frequency wasonce increased to 110Hz, but specimens showed a trendof over heating, so the frequency was settled down to100Hz. Even at that frequency, the total beam energy was
7.0kW in several cm2 that can compare with the heat flux
on divertor in the fusion reactor ITER which is planed as
10MW/m2. This irradiation system got over this high heat
flux and achieved reliable irradiation at around 550℃.
The irradiation damage induced by the electron irradiation is calculated. For the most ceramics, 2.82×1020
electrons in 2cm2 accelerated to 32MeV induces defects
up to 1.00 × 10-2dpa (target mass M=16amu, atomic
number Z=8, knock on energy Ed=30eV). W is far heavier (M=183.8amu) and knock on energy is larger(Ed=100eV), but the collision cross section is 48.4barn
while ceramics shows only 18.7barn. It is said that the Edof W is a little smaller, and if it is 80eV, the cross section
is 60.1barn. Therefore, induced damage in W is larger
than typical ceramics, 1.48×10-2dpa (Ed: 100eV) ～1.95
×10-2dpa(Ed: 80eV).
After the irradiation, radio-activity of the specimen
holder and specimens was investigated. The whole irradiation holder showed over 100mSv/h in the surface at 17h
after the beam stop, 55mSv/h at 33h and 38mSv/h at 40hthat corresponds t1/2 = 13.7h. The half-time of W-185 is
75.1day and W-187 is 23.7h while Cu-64 is 12.7h, so themost of the activity was assumed to be arisen from
Cu-64.

EXPERIMENTS:
In the previous work, 30MeV electron accelerator
KURRI-Linac is used to induce point-defects in bulk
specimens of typical structural ceramics to 1.5x1024e/m2
which correspond to 0.01dpa in typical ceramics. The
irradiation was performed in a new irradiation systemconstructed to achieve an irradiation at around 400℃
where interstitial atoms have enough mobility to migrate.
In the previous work, ceramic specimens were irradiatedusing this irradiation system. In the system, a specimen issettled in a Cu specimen-holder, and holders are piled
between Cu heat spread plates and graphite heat spreadseats. Usually, a graphite seat spreads heat well horizontally, but the graphite seat in this system is `Vertical-Graphite' (produced by Hitachi Chemical) of which
thermal conductivity vertical to the seat is 90W/m・K.
This vertical-graphite sheet was 0.15mm in thickness andwas cut into φ10 that cover the specimen to have goodthermal contact on the surface. In conventional system,
heat contact is achieved by thermal grease that contains
Ag powders. But in this system, neutrons from photo-

採択課題番号 26P6-5
電子線照射後セラミックス中の欠陥評価
プロジェクト（京大・工）秋吉 優史、高木 郁二（京大・原子炉）義家 敏正、徐 虫L、佐藤 紘一
28

PR6-6

The Development of New Positron Beam System Using KUR

Y. Nagai, K. Inoue, T. Toyama, Y. Shimizu, K. Nagumo,
M. Shimodaira, T. Hirota, K Sato1, T. Yoshiie1, Q. Xu1

blocks. After passing the bends, the slow positrons aretransported to sample chamber at an energy up to 20 keV.

Institute for Materials Research, Tohoku University,
1
Research Reactor Institute, Kyoto University

INTRODUCTION: Positron annihilation spectroscopy
is well-known to be a powerful to detect vacancy-type
defects. In 2000 years, it is found that the positron is also
sensitive to (sub)nano embedded particles (SNEPs) withhigher positron affinities than that of the host, even if the
SNEPs are free from open-volume defects. The representative case is ultrafine Cu precipitates in Fe.
We are developing a new positron annihilation apparatus, positron age-momentum correlation (AMOC), tostudy the correlation between the Cu precipitates and thevacancy-type defect induced by neutron irradiation in thelight water reactor pressure vessel (RPV) steels, which isimportant to understand the irradiation induced
embrittlement of the RPV steels due to long-term
in-service exposure to neutron irradiation. For this study,
an intense positron source is required to achieve higher
count rates because typically it takes more than one week
for one spectrum by the conventional AMOC system using 22Na positron source.
In this work, a new positron beam facility with highpositron intensity is constructed at the Kyoto University
Research Reactor (KUR), which is the first reactor based
positron beam in Japan[1].
EXPERIMENTS and RESULTS: An in-pile positronsource was installed at the B-1 hole (20 cm in diameter)
in KUR. The positron beam line consists of two parts:
one is located inside the reactor, and the other is locatedoutside the reactor as shown in Fig. 1 [1,2]. Positrons are
generated by pair production from high-energy γ-rays.
The γ-ray flux and the thermal neutron flux at the positron source position are about 1.5×1012 n/cm2 and 105
Gy/h, respectively, at 5 MW. A W converter of 1 mm
thick and 3 cm diameter and W moderators with a Cd
shroud are used to obtain slow positrons as shown in Fig.
2. In order to enhance the positron generation, a 1 mm
thick Cd shroud covered with an Al plate was mounted
on the top of the magnetic field to cap the converter andmoderator, because high energy γ-ray are generated by
the 113Cd(n, γ)114Cd reaction. The moderators were annealed after the W strips were set in lattices. When annealing, they were encased in covered boxes of 50
μm-thick W foil and the boxes were irradiated on the
covering lids with electron beam welder at KEK in Tsukuba [3]. The annealing temperature was elevated to approximately 2400℃. The vacuum of the welder chamber
was about 10-5 torr. The slow positrons emitted from themoderator were subsequently accelerated up to 30 eV andconfined magnetic fields of several mT. In order to eliminate the background of fast neutrons and γ-rays from thereactor core, the slow positron beam passes two bends inshields consisting of polyethylene, concrete and lead

Figure 1: A schematic diagram of KUR positron
beam system [1,2].

Figure 2: A schematic diagram of the in-pile positron source at KUR [1,2].
Figure 3 shows the positron beam spot recorded using
a microchannel plate (MCP). The beam has a slightly
elliptical shape and the major and minor axes have length
about 2.0 and 1.5cm, respectively. The lattice structure of
W moderator is clearly visible. The positron beam intensity is determined about 106 e+/s at 1 MW by Ge detector.

Figure 3: The observation of positron beam from
KUR using microchannel plate.
REFERENCES:[1] Q Xu et al, J. Phys. Conf. Ser. 505 (2014) 012030.
[2] K Sato et al, Nucl. Inst. Meth. Phys. Resear. B 342(2015) 104.
[3] K Wada et al, Eur. Phys. J. D 66 (2012) 37.

採択課題番号 26P6-6
KUR を用いた新しい陽電子源の開発と材料研究への応用
プロジェクト（東北大・金研）永井康介、井上耕治、外山健、清水康雄、南雲一章、下平昌樹、廣田太一（京大・原子炉）義家敏正、徐虬、佐藤紘一
29

PR6-7

Radiation Damage in Bulk Amorphous Alloys by Electron Irradiation

F.Hori, K.Ishii, T.Ishiyama, K.Kobayashi, A.Iwase,
Y.Yokoyama1, Q.Xu2 and K.Sato2

RESULTS: The mean positron lifetime τ of all
as-quenched sample was about 165 2 psec. Before
irradiation, no difference of positron lifetime for different
amorphous alloy systems was observed. This shows that
open volume existing in amorphous is apparently same.
However, the CDB spectra of these alloys before
irradiation are not necessarily same. Take into account forthese facts, it can be deduced that total electron density ofopen volume in any amorphous alloy is almost same but
the real size of open space and chemical ratio around it
depending on alloy composition is not same for various

Dept. of Mater. Sci., Osaka Prefecture University
2
Institute of Materials Research, Tohoku University
1
Research Reactor Institute, Kyoto University
INTRODUCTION: Bulk amorphous alloys are
expected to be useful for various applications because
they have superior mechanical properties such as
strength, hardness and corrosion resistance. We havebeen suggested that the properties of bulk glassy alloys
can be improved by high energetic particles irradiation.
So far, we have reported that effects of free volume
and mechanical properties on the bulk amorphousalloys depend upon the irradiation species [1,2]. Alsochange in free volume by the irradiation strongly reflects
various properties such as hardness and ductility of bulk

compositional alloys. Figure 1 shows the change inpositron annihilation lifetime by electron irradiation as
a function of Zr composition ratio in bulk amorphousalloys. It found that the increasing trend of positron

lifetime becomes smaller with increasing of Zr
contents. Especially, we found that radiationinduced open volume change is suppressed in glassy
alloys including more than 60% Zr atoms.

amorphous alloys. Recent years, eutectic ZrCuAl bulk
glassy alloy shows the degradation of ductility andtoughness by annealing but that for hypoeutectic
remains unchanged after annealing. In order toestimate irradiation effects for various compositionalbulk amorphous alloys, we performed electron
irradiation for various kinds of ZrCuAl bulk amorphousalloys. Before and after irradiation, we have examined
X-ray diffraction, differential scanning calorimetry (DSC)
and positron annihilation.
EXPERIMENTS: ZrxCu90-xAl10 (x=50, 55, 60, 65)bulk amorphous alloys with 8 mm in diameter and 60 mm
in length were prepared by a tilt casting technique. For
positron annihilation measurements, alloy samples were
cut into the size of about 0.5 mm thickness disk. 8 MeV
electron irradiations with total dose of 2x1018 e/cm2 was
performed for these alloys at 320 K by LINAC at
Research Reactor Institute, Kyoto University. During
irradiation, samples were cooled in water flow path.
Irradiated samples were examined by X-ray diffraction,
positron annihilation lifetime and coincidence Doppler
broadening measurements at room temperature. The
positron annihilation lifetime spectra consist of more than
1.0 x 106 counts. The positron lifetime spectra wereanalyzed by using POSITRONFIT program.

Fig. 1 Change of positron lifetime for various compositions of
ZrCuAl bulk amorphous alloys by 8 MeV electron irradiation.
REFERENCES[1] N.Onodera, A.Ishii, Y.Fukumoto, A.Iwase, Y.Yokoyama,
and F.Hori, Nucl. Inst. & Meth. B. 282 (2012) 1[2] F.Hori, N.Onodera, A.Ishii, Y.Fukumoto, A.Iwase,
A.Kawasuso, A.Yabuuchi, M.Maekawa and Y.Yokoyama, J.
Phys.: Conf. 262 (2011) 012025

	
 採択課題番号 26P6-7	
 金属合金における照射効果の研究
	
  	
  	
  	
 
	
 
プロジェクト
（阪府大・工）堀史説、石井康嗣、石山大志、小林一基、岩瀬彰宏、（東北大・金研）横山嘉彦	
 	
 (京大・原子炉)徐虫 L	
 、佐藤紘一	 30

PR6-8

Positron Annihilation Study of Fe-Cr Alloys after Neutron Irradiation in KUR

R. Kasada1, K. Sato2, Q. Xu31018 n/cm2). Positron annihilation lifetime spectrometry
was carried out for investigating open-volume type defects produced by irradiation.

1

Institute of Advanced Energy, Kyoto University
Department of Mechanical Engineering, Kagoshima
University
3
Research Reactor Institute, Kyoto University

2

Results and Discussions: Results of positron annihilation lifetime spectrometry is shown in Table 1. There isno meaningful difference in the mean lifetime of unirradiated Fe-Cr binary alloys. After the neutron irradiation
in KUR, the mean lifetime of pure Fe and Fe-xCr alloys
for x ≤ 85 slightly increased but not decomposed into
multi-components. On the other hand, that of Fe-91Cr
and pure Cr showed two- and three components, respectively. This results indicate that Fe atom suppress vacancy cluster formation in the Fe-Cr binary alloys from aview of the Cr-rich side. Further investigation is needed
for understanding the effect of Cr (or Fe) atom on theformation of vacancy type cluster in Fe-Cr alloys.

INTRODUCTION: Ferritic steels containing Cr are
expected to be used for the first-wall component of thefusion reactors as well as for the fuel pin cladding of theGeneration IV nuclear fission systems [1]. However,high-Cr steels may suffer from thermal aging embrittlement, which is well-known 475 °C embrittlement. This ismainly due to hardening phenomenon through the phaseseparation of Fe and Cr as shown in the phase diagram.
In the previous study [2], we applied a positron annihilation spectrometry to detect the phase separation in the
Fe-Cr alloys after thermal aging at 475 °C.
The present collaborative research has investigate theneutron irradiation effect on the positron annihilation
lifetime of Fe-Cr alloys.

REFERENCES:[1] A. Kimura, et al., Journal of Nuclear Science andTechnology, 44 (2007) 323-328.
[2] R. Kasada and K. Sato, submitted to J. Alloys andCompounds.

Experimental Procedure: Materials used in the present
study are Fe-xCr binary alloys. Neutron irradiation onthese materials was carried out at 300 °C up to 199 h in
KUR. The displacement damage is 2.1 × 10-3 dpa (5.1 ×

Table 1 Results of positron annihilation lifetime spectrometry of Fe-Cr
alloys before and after neutron irradiation in KUR.
Materials
Fe
Fe-9Cr
Fe-15Cr
Fe-30Cr
Fe-45Cr
Fe-50Cr
Fe-70CrFe-85Cr
Fe-91Cr
Cr

Unirr.
τm (ps)104 ± 1
107 ± 1105 ± 1105 ± 1105 ± 1105 ± 1105 ± 1104 ± 1105 ± 1103 ± 1Irr.
τ1 (ps)109 ± 1109 ± 1109 ± 1109 ± 1109 ± 1108 ± 1
107 ± 1110 ± 1113 ± 124 ± 4I1 (%)

τ2 (ps)I2 (%)

τ3 (ps)I3 (%)

93 ± 19±1383 ± 9156 ± 27±1
48 ± 1502 ± 343 ± 1

採択課題番号26P6-10
鉄クロム系合金の相平衡に及ぼす照射影響
プロジェクト（京大・エネ理工研）笠田竜太（鹿児島大・理工）佐藤紘一（京大・原子炉）徐虬

31

PR6-9Positron Annihilation Lifetime Measurements of Austenitic Stainless Steels
Irradiated in the SINQ Target Irradiation Program

K. Sato, Q. Xu1, T. Yoshiie1, Y. Dai2 and K. Kikuchi3

100 K from 423 to 1323 K. After annealing, samples
were cooled down by air cooling. Cool time to room
temperature was about 20 minutes.

Graduate School of Science and Engineering, Kagoshima
University
1
Research Reactor Institute, Kyoto University
2
Spallation Neutron Source Division, Paul Scherrer Institut
3
Frontier Research Center for Applied Atomic Sciences,
Ibaraki University

RESULTS: Short and long lifetime component in thetwo component analysis was 150 (6) ps and 237 (7) ps,
respectively. Intensity of short and long lifetime component was 49 (7) % and 51 (7) %, respectively. Errors areshown in parentheses. The long lifetimes result from theformation of vacancy-cluster–He-atom (Vm-Hen) complexes (large open space defects), while the short lifetimes denote the formation of stacking fault tetrahedra(SFTs), dislocation loop, and single-vacancy–He-atom(V-Hen) complexes (small open space defects). The experimental value of 230 ps is slightly smaller than thecalculated positron lifetime of 249 ps for 4-vacancy clusters (V4) in Ni. Yet the vacancy cluster size is not likely
to be less than 4, because many He atoms formed in thesamples during irradiation. The positron lifetime of the
He bubbles decreases as the number of He atoms in avacancy cluster increases. Thus the exact vacancy cluster
size cannot be determined, because they are too small tobe directly observed by TEM.
The positron lifetime does not change after isochronal annealing up to 623 K. The spectra only show one
component for annealing between 723 and 923 K, butthey resolve into two components when annealed above
1023 K. It is expected that Vm-Hen complexes absorb He
atoms by annealing at temperatures up to 623 K. Because
the complexes incorporate many He atoms after irradiation, the lifetime decrease caused by absorption of helium
may become saturated. In this stage, the He bubble concentration does not change because the long lifetime intensity is almost constant. SFTs and V-Hen complexes are
expected to dissociate after annealing at 623 K. These
defects, which have a short lifetime for annealing at up to523 K, tend to aggregate and Vm-Hen complexes areformed. It is impossible to resolve them into two components. A small increase in the mean lifetime arises because of both the growth of Vm-Hen complexes and theirrelease of H atoms. The Vm-Hen complexes dissociate
after annealing at 1023 K. In this stage, the absorption ofvacancies is larger than that of He atoms, and therefore,
the long lifetime increases.

INTRODUCTION: Austenitic stainless steels havebeen known as highly corrosion resistant materials andimportant nuclear materials. There have been a number ofstudies on the void swelling behavior of them [1,2]. Recent theoretical and experimental analyses have revealed
the importance of incubation period, a transient stage
before the steady growth of voids. However, experimental results of void swelling in austenitic stainlesssteels have been limited to high dose. Because most ofexperimental studies have been performed by transmission electron microscopy after observable void formation,and point defects and their clusters under the resolution
limits are impossible to detect. Therefore, point defectprocesses during the incubation period are not clear. In
this study, the effect of alloying elements on defectstructures in austenitic stainless steels and their model
metals during the incubation period was studied after
neutron irradiation by using positron annihilation lifetime
measurement.
EXPERIMENTS: Titanium-doped 316-type austenitic
stainless steel, called Japanese Primary Candidate Alloy(JPCA), and the reduced activated ferritic/martensitic
steel F82H were used in this study. The JPCA was irradiated in the first SINQ (Swiss Spallation Neutron Source)
target irradiation program (STIP-I). More details of the
STIP-I experiments have been previously reported [3].
Irradiation position was F21. Irradiation temperature was
413K, and irradiation dose was 6.3dpa. After implementing a fatigue test on JPCA at room temperature, the positron annihilation lifetimes of the undeformed area of thesample were measured at the Research Reactor Institute,
Kyoto University. A three-detector system using a fast
digital oscilloscope and BaF2 scintillators [4] was adopted for the positron annihilation lifetime measurements,
thereby reducing the background counts and making it
possible to measure highly radioactive samples. The time
resolution of the system was 150 ps (full width at half
maximum). Each spectrum was accumulated to a total of
1.5 × 106 counts. The resulting spectra were analyzed
using the PALSfit program [5]. The isochronal annealingof the positron annihilation lifetime was examined every

REFERENCES:[1] F.A. Garner, Materials Science and Technology, Vol.
10 (VCH Weinheim, 1994), p. 419.
[2] T. Okita et al., J. Nucl. Mater. 307−311 (2002) 322.
[3] Y. Dai and G.S. Bauer, J. Nucl. Mater. 296 (2001) 43.
[4] H. Saito et al., Nucl. Instr. Meth. Phys. Res. A 487(2002) 612.
[5] J.V. Olsen et al., Phys. Stat. Sol. C 4 (2007) 4004.

採択課題番号 26P6-12 電子照射と中性子照射によって形成した金属中の格子欠陥と プロジェクト
ガス原子の相互作用の解明（鹿児島大院・理工）佐藤紘一（京大・原子炉）徐虬、義家敏正（九大・応力研）大澤一人（産総研）大島永康
32

PR6-10 Effects of High Energy Particle Irradiation on Hydrogen Retention in Refractory Metals
K. Tokunaga, M. Matsuyama1, S. Abe1, H. Osaki2, K.
Araki, T. Fujiwara, M. Hasegawa, K. Nakamura, Q. Xu3
and K. Sato3

gas was about 5 %. Temperatures of pre-heating and T
exposures were 100 oC. After the exposure to T gas, T
amount retained in surface layers of the sample was
evaluated by -ray-induced X-ray spectrometry (BIXS)
and imaging plate (IP) measurements.

Research Institute for Applied Mechanics, Kyushu University
1
Hydrogen Isotope Research Center, University of Toyama
2Interdisciplinary Graduate School of Engineering Sciences, Kyushu University
3
Research Reactor Institute, Kyoto University

RESULTS: Temperature of the W samples during theelectron irradiation was 85 oC. Figure 1 shows the resultof the IP measurement of ITER grade W(1) (IG W(1))
and ITER grade W(3)(IG W(3)). The IP images indicatethat amount of T on the surface of IG W(3) is larger thanthat of the surface of IG W(1). Comparison with thestandard samples shows that amount of T of the surfaceof IG W(1) and IG W(2) are 0.0604 kBq/mm2 and 0.166
kBq/mm2, respectively. Figure 2 show line analyses of
PLS value of the surface of IG W(3) (a) and IG W(1) (b)after the T exposure. It can be seen that line profiles arealmost constant. These result indicates that T is easy todiffuse parallel direction for rolling direction. Electron
beam irradiation effect will be discussed by comparing
with the result of un-irradiated W samples.

INTRODUCTION: It is of importance to clarify phenomena of implantation, retention, diffusion and permeation of tritium on surface of the armor materials of thefirst wall/blanket and the divertor on fusion device from aviewpoint of precise control of fuel particles, reduction oftritium inventory and safe waste management of materials contaminated with tritium (T). Refractory metals suchas tungsten (W) is potential candidate for an armor of thefirst wall and the divertor plate of the fusion reactor because of its low erosion yield and good thermal properties.
The armor material will be subjected to heavy thermalloads in the steady state or transient mode combined withhigh energy neutron irradiation that will cause serious
material degradation. In addition, high energy runaway
electrons would bombard the armor materials along theequatorial plane in fusion device. It is considered thatthese cause radiation damage and enhance tritium retention. In the present works, T exposure experiments havebeen carried out on W samples which were irradiated byhigh energy electrons using LINAC in KURRI of Research Reactor Institute, Kyoto University to investigate
effects of high energy electrons irradiation and microstructure on tritium retention of W.

Fig. 1. Tritium image of ITER grade W(3) (IGW(3) and ITER grade W(1)(IG W(1). Bottom parts
are standard samples.

PLS/hr

PLS/hr

EXPERIMENTS: W samples used in the present experiments were two oriented ITER grade W. One was W
sample (ITER grade W(1)) which the surface were manufactured to be oriented parallel to the rolling surface androlling direction. The other was W sample (ITER grade
W(3)) which the surface were manufactured to be oriented perpendicular to the rolling surface and rolling direction. The sizes of W samples were 10mm x 10mm x
1mm. The surface of the both samples were polished tobe mirrored． High energy electrons irradiation has been
carried out using LINAC in KURRI of Research Reactor
Institute, Kyoto University. An energy of electron irradiated was 10 MeV and DPA was 3.26 x 10-3. Temperatureduring the irradiation was measured by thermocouples
which was contacted with a backside of the W samples.
After the electron beam 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 concentration in the

0.014
0.012
0.010
0.008
0.006
0.004
0.002
0.000

0.014
0.012
0.010
0.008
0.006
0.004
0.002
0.000

IG W(3)

(a)

0

2

4
6
8
Position (mm)12IG W(1)

(b)

0

10

2

4
6
8
Position (mm)1012Fig. 2. Line analyses of IG W(3) (a) and IG W(1) (b)after tritium exposure.

採択課題番号 26P6-13

高融点金属における水素吸蔵特性に及ぼす
プロジェクト高エネルギー粒子線照射効果（九大・応用研）徳永和俊、荒木邦明（九大・総理工）尾崎浩詔（京大・原子炉） 徐 虬、佐藤紘一

33

PR6-11

Depenedence of Cellular Structure Formation on Ion Species

N. Nitta1, C. Watanabe1, M. Taniwaki1, Q. Xu2, T.
Yshiie2
1School of Environmental Science and Engineering,
Kochi University of Technology
2
Research Reactor Institute, Kyoto University
INTRODUCTION: Fine cellular structure is formed on
GaSb, InSb and Ge semiconductors by ion irradiation asshown by Fig. 1[1]-[6]. The authors proposed an idea that
this structure is formed by the behavior of point defects
induced by ion irradiation, that is, first the voids form
from the oversaturated vacancies and they develop byabsorbing point defects induced continuously during ion
irradiation. This idea has been proved by intense studies
on the ion dose dependence and temperature dependenceof the cellular structure. However, the authors do nothave detailed understanding over all the cell formation
process. Especially, the details of the formation mechanism of voids are not yet clear. Though the authors havesurely observed the voids prior to the development of thecellular structure, the diameter of these voids are so large(30-50 nm) and the smaller voids are not yet found, thenlarge voids appear suddenly during ion irradiation, notdeveloping from small voids. Therefore another effect on
voids formation, for example, the thermal spike, is suspected. Thermal spike effect depends on the mass of ions,then, the authors aim to investigate the ion mass dependence of the voids formation and development in this work.
In addition, the chemical effect of implanted ions is studied.

100nm
Fig. 1. FE-SEM image of GaSb surface by 60
keV Sn+ implanted GaSb to a dose of 1.2  1015
ions/cm2 at 150 K.
irradiated sample have small diameters less than 30 nm,
but some of the voids (the density is about 2/1 m2) haveabout 100 nm diameter. These relatively large voids are
removed their top surfaces but seem to consist of single
void.
In Si irradiated wafer, some small contrasts which mightshow the voids were observed, and their density was
about 2/1m2. However, in Al ion irradiated samples, thevoid contrast was not observed. These atom masses are sosmall (26.98 and 28.09) that the ion range is large anddistribution is wide, therefore it is considered that the
point defects density is too small for voids formation anddevelopment.
By SEM study which has been performed until now, it
was assured that the atomic mass of irradiated ion affects
the voids formation and development. However, from
SEM study we cannot know much under the surface, then,the details are not yet clarified. The authors will study
under the surface by cross-sectional TEM in order to understand the void formation mechanism.

EXPERIMENTS: The GaSb (001) wafers were implanted by C, Si, Ge, Pb (IV elements as Sn), Al and P
ions by accelerated by 60 kV voltage to the dose of 10 15
ions/cm2. The wafers were kept at 100-110 K during ion
irradiation. The surface morphology of the implanted
wafers was observed by a FE-SEM.

REFERENCES:[1] 新田紀子, 谷脇雅文, 鈴木朝夫, 林 禎彦, 佐藤
裕 樹 , 義 家 敏 正 , 日 本 金 属 学 会 誌 , 64 (2000),
1141-1147.
[2] N. Nitta, M. Taniwaki, T. Suzuki, Y. Hayashi, Y. Satohand T. Yoshiie, Materials Transactions, 43 (2002),
674-680.
[3] N. Nitta, M. Taniwaki, Y. Hayashi and T. Yoshiie, J.
Appl. Phys., 92 (2002), 1799-1802.
[4] N. Nitta, M. Taniwaki, Y. Hayashi and T. Yoshiie,
Physica B, 376-377 (2006), 881-885.
[6] N. Nitta, T. Hasegawa, H. Yasuda, Y. Hayashi, T. Yoshiie, and M. Taniwaki, Materials Transactions 52,(2011) 127-129.

RESULTS: Voids removed their top surfaces were observed on the relatively large mass ions (Ge and Pb) irradiated wafer surfaces, and they were scarcely formed thesmall mass ions (Si and Al) irradiated surfaces.
In the case of Pb with the largest atom mass (207.2), thediameter of voids was widely distributed from 10 nm 300 nm. The density of voids with a diameter of 100 nm
and over are 4.4/1 m2, and they are formed by coalesceof neighboring voids (these void diameters are less thanabout 100 nm), consequently, the maximum diameter ofindividual voids is 100 nm at most.
Most of the voids observed in Ge (atomic mass =72.64)

採択課題番号 26P6-14
化合物半導体のイオンビーム照射効果（高知工科大・環境）新田紀子、谷脇雅文（京大・原子炉）徐 虬、義家敏正
34

プロジェクトPR8Development on Neutron Imaging Application

Y. Saitoframe rate neutron radiography to measure the film
thickness distribution.
ARS-2 applied neutron radiography to heat transfer
study on an adsorption refrigerator. In this ARS, visualization of adsorption amount distributions of ethanol in an
activated carbon powder bed, using Umbra method inneutron radiography.
ARS-3 visualized the flow in a tubular flow reactor for
supercritical hydrothermal synthesis of nanoparticle using neutron radiography. Measured mixing behaviors in
the tubular flow reactor were compared with the size
distributions of the synthesized nanoparticles.

Research Reactor Institute, Kyoto University
1. Objectives and Allotted Research Subjects
Neutron imaging provides valuable information whichcannot be obtained from an optical or X-ray imaging. The
purpose of this project is to develop the imaging method
itself and also the experimental environment for expanding the application area of the neutron imaging. The allotted research subjects are as follows:
ARS-1 Measurements of Multiphase Dynamics by Neutron Radiography (Y. Saito et al.)ARS-2 Quantitative Measurement of Adsorbed Ethanol
Amount in Activated Carbon Adsorber for Adsorption Heat Pump (N. Takenaka et al.)
ARS-3 Neutron Radiography on Tubular Flow Reactor
for Supercritical Hydrothermal Synthesis of
Nanoparticles (T. Tsukada et al.)
ARS-4 Characteristics of the Void Fraction under Transient Condition (H. Umekawa et al.)
ARS-5 Neutron imaging and optics development using
simulation of VCAD Systems (Y. Yamagata etal.)
ARS-6 Water and Salt Distribution in a Rice Hull Medium under Sodium Chloride Solution Culture(U. Matsushima et al.)
ARS-7 Measurement of Water Content in Hardened
Cement Paste by Neutron Imaging (T. Numao et
al.)
ARS-8 Hydrazine Thickness Measurement by NeutronRadiography at a Catalyst Bed during Operation(H. Kagawa et al.)
ARS-9 Development of Neutron Imaging Devices (H.
Iikura et al.)
ARS-10 Evaluation of the Moisture Movement in
High-Performance Concrete Subjected to Heating (M. Kanematsu et al.)
ARS-11 Effect of gravity on coolant distribution in
FGHP heat spreader (K. Mizuta et al.)
ARS-12 Study on Visualization of Organic Materials
between Metals for Advance of Industrial Products (A. Uritani et al.)
ARS-12 Study on Visualization of Organic Materials
between Metals for Advance of Industrial Products (A. Uritani et al.)
ARS-13 Visualization of Flow inside Fine Scale of Heat
Pipe (Y. Tsuji et al.)

ARS-4 was not performed this year.
ARS-5 was trying to develop a visualization techniquefor molding process by using neutron radiography andalso a neutron focusing mirror. A 100mm rotational ellipsoid mirror was fabricated and its focusing performance was investigated at the CN-3 port
ARS-6 was not performed this year.
ARS-7 was not performed this year.
ARS-8 was not performed this year.
ARS-9 was not performed this year.
ARS-10 evaluated the water distribution in the hardened cement paste (HPC) using neutron radiography. In
this study, experiments were carried out to investigate
two-dimensional moisture movement in HPC.
ARS-11 applied neutron radiography to observe coolant distributions in a flat heat spreader (FGHP). The effect of gravity on coolant distribution in the FGHP wasinvestigated by varying the heat load to the FGHP. At
present experimental conditions, at least 0.1 mm thickliquid layer in the wick area exists in the middle plates of
the FGHP.
ARS-12 applied neutron radiography to observe organic materials between metals for advance of industrial
products. Experiments were conducted at the E-2 port
and the test samples were bearing with and without
grease. From the CT reconstruction of the neutron images,
the grease distributions could be clearly observed.
ARS-13 applied neutron radiography to observe working fluid distributions in a house-made heat pipe, to understand the heat transfer process on a solid surface. Experiments were conducted at the E-2 port, and the heatpipe was visualized by changing he heat load from 6W to
30W. Cross sectional distributions of the working fluid
could be measured by the neutron radiography.

2. Main results and the contents of this report
In ARS-1, simultaneous measurements of water film
distribution in an air-water two-phase flow were performed by using a Liquid Film Sensor (LFS) and a high

採択課題番号 26P8
（京大・原子炉）齊藤泰司

中性子イメージングの高度化と応用

35

プロジェクトPR8-1

Dynamic Observation of Two-Phase Flow using Neutron Radiography

Y. Saito and D. Ito
Research Reactor Institute, Kyoto University
INTRODUCTION: Neutron radiography (NRG) is a
powerful tool for fluid flow visualization as well as
two-phase flow research. Gas-liquid two-phase flows in a
metallic pipe have been visualized clearly by using NRG.
However, it would be still difficult to obtain dynamic
information on such flows by NRG, because of insufficient neutron flux from neutron sources and poor efficiency of imaging devices. In this work, our imaging
system was improved and a denoising method for acquired image sequence was developed for high frame rate
NRG. Then, they were applied to air-water two-phaseflow measurements in a narrow rectangular channel. In
addition, a simultaneous measurement with an electricalconductance method was performed to investigate thedetailed structure of the two-phase flow.

Fig. 1. High frame-rate neutron radiography systema

EXPERIMENTS: Experiments were performed at theB-4 supermirror neutron guide facility [1] of the Research Reactor Institute, Kyoto University. The neutron
flux of the B-4 port is 5×107 n/cm2s and the beam widthand height at the beam exit are 10 mm and 75 mm, respectively. An imaging system for high frame rate NRG
consists of a neutron converter, a dark box with a single
mirror, a megapixel lens, an image intensifier and a highspeed camera, as shown in Fig.1. NRG images acquiredby this system were used to estimate the void fraction in
the channel gap. Since the measured data include severe
signal noises due to the statistical error in counting neutrons, a spatio-temporal filter was applied to enhance thequality of the void fraction distributions [2].
The test section has a rectangular cross section with 12
mm width and 2 mm gap. The vertical channel wasplaced at 1 m away from the neutron beam exit. The test
fluids are air and tap water at room temperature. A liquidfilm sensor (LFS) [3] based on an electrical conductancemeasurement was applied to visualize the water film
flowing in the narrow channel, which was installed on
one side of the channel walls. LFS has 7×32 measurement points and the distance between the points was 1.5
mm. The temporal resolutions of both measurements
were 200 Hz for NRG and 10,000 Hz for LFS.

b

c

d

Fig. 2. Measured and filtered results of void fraction distribution

Thickness [m]

2000

1500

bubble thickness (NRG)
film thickness (LFS)
film thickness (estimated)

1000

500

0

3

6

9

12

Distance [mm]Fig. 3. Bubble and liquid film thickness profiles
The typical results obtained by a simultaneous measurement with NRG and LFS were shown in Fig.3. The horizontal profiles of the bubble and film thicknesses are
represented. It is seen that the bubble occupies most of
the gap in the channel. Thin film on the LFS could bemeasured by LFS. The film thickness on the opposing
wall, which was estimated from the measured data of
NRG and LFS, is also plotted in Fig. 3. This thickness
profile agreed well with LFS result. Thus, the possibilityof liquid film measurement on another wall was shownby the hybrid measurement with NRG and LFS.

RESULTS: The typical void fraction distributions
measured by NRG are shown in Fig.2 (a) and (b). Highvoid fraction values indicate where the bubble exists, andthe size of bubbles could be roughly estimated from the
distribution. However, several signal noises were found
not only in the liquid phase region but also in the gas
phase. Thus, the 3-D non-local mean filter was applied tothe original images. The distributions filtered from Fig.2(a) and (b) are shown in (c) and (d), respectively. The
remarkable noises were reduced by the filtering process.

REFERENCES:[1] Y. Saito, et al., Nucl. Instr. Meth. Phys. Res., A, 651(2011) 36-41.
[2] Y. Saito and D. Ito, Proc. WCNR-10, (2014).
[3] D. Ito, et al., Exp. Fluids., 51-3 (2011) 821-833.

採択課題番号 26P8-1 中性子ﾗｼﾞｵｸﾞﾗﾌｨを用いた混相流のﾀﾞｲﾅﾐｯｸｽ計測に関する研究（京大・原子炉）齊藤泰司、伊藤大介
36

プロジェクトPR8-2

Quantitative Measurement of Adsorbed Ethanol Amountin Activated Carbon Adsorber for Adsorption Heat Pump

H. Asano, K. Murata, N. Takenaka, H. Murakawa, K.
Sugimoto, Y. Saito1, D. Ito1, Y. Kawabata1

relationship could be obtained for the adsorbed ethanolby the umbra method as plotted with the symbol of ●.
The measured values by neutron radiography wascompared with those reported by El-sharkawy et al. [2] inFigure 7. They proposed the Dubinin–Astakhov equation
for adsorbed ethanol amount on the same activatedcarbon based on the experimental results. It was
confirmed that the adsorbed refrigerant amount could bemeasured quantitatively by the neutron radiography.

Department of Mechanical Engineering, Kobe University
Research Reactor Institute, Kyoto University

1

INTRODUCTION: Adsorption refrigerator is one of
the efficient tools to recover waste heat at a lowtemperature. A design of the adsorber, in which
refrigerant is adsorbed in adsorbent particle bed, is a key
part for the improvement in the performance. To design
the configuration of adsorber, it is required to clarify theadsorbed refrigerant distribution in the adsorbent particle
bed during adsorption/desorption process. Neutron
radiography was applied to visualize the adsorption
amount distribution of ethanol in an activated carbon
particle bed. The umbra method was applied tocompensate the neutron scattering effect for quantitative
measurement.

3 mm x 3 mm checked grid
Measured area
50×50 pixel
Neutronabsorber
Observed area

Fig. 1 Neutron absorber grid for umbra method.
With the cmpensation by the umbra method
Liquid ethanol
Adsorbed ethanol
Without the compensation
Adsorbed ethanol
2.5
2.0

r m,r r [-]EXPERIMENTS: Activated carbon and ethanol wasused as the adsorbent and refrigerant, respectively. The
activated carbon MAXSORB® III produced by Kansai
Coke and Chemical co., ltd. was used as the adsorbent. At
first, the mass attenuation coefficient of liquid ethanol
was measured using an ethanol step. Then, quantifiability
in the measurement of adsorbed ethanol amount in
activated carbon particle bed was evaluated by themeasurement of an adsorbent step in dry and adsorption
equilibrium condition. The adsorbent temperature was
21.5 °C and the pressure was 4.09 kPa. The umbra
method using neutron absorber was applied to thequantitative measurement. A checked neutron absorber
grid shown in Fig.1 was newly made for two-dimensional
measurements. The offset value for an observed area canbe measured by interpolating the brightness at theposition covered by the neutron absorber surrounding theobserved area. The width of the grid was 3 mm.

1.5
1.0
0.5
0

0
5
10
15
20
25
Thickness of the adsorbent/ethanol step [mm]rr [g/cm2]

Adsorption amount in equibribrium
by El-sharkawy et al. (2008)

Fig. 2 Attenuation of neutron beam for various thickness of the adsorbent or ethanol step.

RESULTS: The measured results of the liquid methanol
step are plotted with the symbol of ▲ in Fig. 2. The
vertical axis shows the product of density, , massattenuation coefficient, m, and thickness along theneutron beam, . The subscript r means ethanol as therefrigerant. A liner relationship between ethanol
thicknesses and rm,rr could be successfully obtained.
The mass attenuation coefficient calculated from thegradient was 3.86 cm2/g. For the measured results ofadsorbed ethanol without the compensation plotted withthe symbol of ○, the values seemed to become saturated
due to the effect of neutron scattering and stray light inthe camera system. It could be seen that the linear

0.6
0.4
0.2
0

0
0.2
0.4
0.6
Adsorption amount measured
by neutron radiographyrr [g/cm2]

Fig. 3 Comparison of adsorption amount in equilibriumwith the calculation by El-sharkawy et al.[2].
REFERENCES:[1] N. Takenaka, et al., Nondestructive Testing and Evaluation, 16-693 (2001), 345-354.
[2] I.I. El-Sharkawy, et al., Int. J. of Refrigeration, 31-8
(2008), 1407-1413.

採択課題番号26 P8-2
中性子ラジオグラフィによる機器内流動の可視化計測
プロジェクト
（神戸大・工）竹中信幸、浅野等、村川英樹、杉本勝美（京大・原子炉）齊藤泰司、伊藤大介、
川端祐司、（神戸大・工）村田健太、中村俊裕、北村信樹、米田久志、澤田将貴、古野正晃
37PR8-3

Neutron Radiography on Tubular Flow Reactor for Supercritical Hydrothermal
Synthesis of Nanoparticles

T. Tsukada, K. Sugioka, M. Kubo, K. Ozawa, S. Takami 1,
T. Adschiri2, K. Sugimoto3, N. Takenaka3, Y. Saito4
and Y. Kawabata4

in supercritical water. The size distribution of nanoparticles in (b) is much broader than those in (a), and the average sizes and the CV values of synthesized nanoparticles in (a) is smaller than those in (b). Here, the average
size of an octahedral particle was defined by (ls)1/2 withthe lengths of major and minor axes, l and s, of particle.
Such size distribution dependence of nanoparticles onreactor configuration is due to the difference in flow andthermal fields in the reactors. As the results of neutron
radiography show, the stream of supercritical waterflowing down through the vertical tube penetrates into
the horizontal tube, and a thermally, density-stratified
layer is generated in the horizontal tube of (a), while itseems from the temperature distributions in (b) that
thermal buoyancy convection occupies the vertical tube
just above the T-junction.

Dept. of Chemical Engineering, Tohoku University
1
IMRAM, Tohoku University
2
WPI-AIMR, Tohoku University3
Dept. of Mechanical Engineering, Kobe University
4
RRI, Kyoto University
INTRODUCTION: Recently, a variety of metal-oxide
nanoparticles have been synthesized by supercritical hydrothermal synthesis [1]. For the design and optimization of the process, it is important to acquire the correctknowledge about the mixing behavior of cold aqueous
feed solution and supercritical water in a hydrothermal
reactor. Therefore, we used neutron radiography to visualize the flow in a tubular flow reactor for supercriticalhydrothermal synthesis, and investigated the effects ofthe flow rates of two fluids and reactor configurations on
the mixing behavior in the reactor [2-4]. In this work,
CeO2 nanoparticles were actually synthesized by supercritical hydrothermal synthesis under the same conditions
as those in neutron radiography, and then the size distributions of synthesized nanoparticles were discussed
comparing with the flow and thermal fields observed byneutron radiography.

CONCLUSIONS: The relationship between the size
distributions of synthesized nanoparticles and the mixing
behaviors of the metal salt aqueous solution and supercritical water in the reactor was clarified by comparing
between the results of supercritical hydrothermal synthesis and neutron radiography in the reactor.
REFERENCES:[1] T. Adschiri et al., Green Chemistry, 13 (2011) 1380.
[2] S. Takami et al., J. Supercrit. Fluids, 63 (2012) 46.
[3] N. Takenaka et al., Phys. Procedia, 43 (2013) 264.
[4] K. Sugioka et al., AIChE J., 60, (2014) 1168.

EXPERIMENTS: The tubular flow reactor, which wascomprised of a Swagelok union tee and SUS316 tubes
whose outer diameter and wall thickness were 1/8 inch
and 0.71 mm, respectively, was used for synthesizing
CeO2 nanoparticles. Two streams of 10 mM Ce(NO3)3
aqueous solution and supercritical water were mixed andreacted at the T-junction in the reactor under approximately 25 MPa. The size distributions and average diameters of synthesized nanoparticles were evaluated using
SEM (S-4800, Hitachi High-Technologies Co., Japan).
Neutron radiography of the tubular flow reactor was
the same as that in our previous works [2-4], where athermal neutron beam emitted from the B4 port in KUR
was used. The imaging method of neutron radiography
and subsequent analysis of the images were also similar
to those in our previous work [3].
RESULTS:
Figures 1 (a) and (b) shows SEM images
and size distributions of nanoparticles synthesized using
tubular flow reactors with two different configurations,when the flow rates of supercritical water and Ce(NO3)3
aqueous solutions were 8.0 and 1.0 g/min, respectively.
In the figures, the temperature distributions obtained byneutron radiography are also shown. Octahedral CeO2
nanoparticles are found to be synthesized hydrothermally

Figure 1 SEM images and size distributions of synthesized nanoparticles, and temperature distributions observed by neutron radiography.

採択課題番号 26P8-3 中性子ラジオグラフィを利用した超臨界水反応場の in-situ 観察 プロジェクト（東北大院・工）塚田隆夫、杉岡健一、久保正樹、小澤恭兵、（東北大・多元研）高見誠一、（東北
大・WPI）阿尻雅文、（神戸大院・工）杉本勝美、竹中信幸、（京大・原子炉）齊藤泰司、川端祐司
38PR8-4

Neutron imaging and optics development using simulation of VCAD Systems

Y.Yamagata*1, S.Morita*1,J.Guo*1, J.Kato*1, H.Yokota*1,
T.Sera*1*2, Y.Kawabata*3, Y. Saitoh*3, M.Hino*3,
M.Sugiyama*3 ,D.Ito*3

RESULTS:
Fig. 1 shows the photo of the ellipsoid mirror through the
manufacturing process. Fig.2 shows the beamline setup
for ellipsoid mirror testing. The beam cam through pinhole (1mm) and U-shaped slit to eliminate the neutron
beams that will not reflect on the mirror surface. The focused beam is detected by RPMT detector. It was possible to detect neutron beam focusing using this small mirror as shown in Fig.3. Focusing performance using
VCAD software will be conducted in the near future.

RIKEN Center for Advanced Photonics, RIKEN*1,
Osaka University*2, Kyoto University Research Reactor
Institute*3

INTRODUCTION:
VCAD System is a cluster of software codes, which cangenerate "real" object model in a computer and perform
various numerical simulation. Those software codes include geometry conversion and input tools, 3D visualization, segmentation and mesh-generation tools, and various FEM-based simulation tools. The authors have been
applied the neutron radiography data to VCAD systems
to generate 3D geometry data and FEM analysis. Those
software also include a simulation code for "real" opticalcomponents. We did a consideration about possible application of neutron radiography for the production process visualization for glass press mold lens and also conducted focusing experiments of small rotational ellipsoid
mirror.

Fig.1 Manufactured ellipsoid mirror (a)aluminum
substrate (b)NiP plated (c)polish finished
L = 2.5 m
PinholeSlit

Chopper
Neutrons

RPMT

EXPERIMENTS:(1)Consideration of visualization of molding process
It was not possible to carry out a neutron radiography,
but we have considered the possibility of neutron radiography to visualization of glass molding process ofaspherical lens. Many lenses for digital cameras today
include at least a few aspherical lenses. Those asphericallenses are manufactured by glass press molding usingtungsten-carbide molding die at very high temperature of
500 to 900 degree. Since the process is done with hightemperature inside tungsten carbide die, it was not possible to visualize the process. Total cross section of tungsten (W) is 23.1 for thermal neutron and considering thatmost glass material contain boron which has very highcross section, it may be possible to visualize the molding
process through tungsten carbide die.
(2) Neutron beam focusing experiment
To manufacture a neutron focusing mirror with relatively lower cost and manufacturing time, the authors
have started the development of neutron focusing mirror
using metallic substrate.[1] The advantage of metallic
substrate are easier mechanical handling and shorter
manufacturing time. A 100mm rotational ellipsoid mirror was fabricated and focusing performance was tested
at CN-3 port.[2]Goniometer stage(6-axis)Ellipsoidal focusing mirror(a=1250, b=7)
Rail

Fig.2 Experimental setup for neutron focusing experimenta. Focusing spotc. 250 mm away from b. mirror-to-detector
mirror center
distance (625 mm )d. Direct beamfrom U slit

Fig.3 Focusing experiment result
REFERENCES:[1] S.Takeda, H.Ohno, H.Sato, M.Furusaka, S.Morita,
Y.Yamagata, M.Hino, "Development of an ellipsoidal
neutron supermirror with metal substrate", International
Workshop on Neutron Optics and Detectors, July (2013)[2] J.Guo, S.Takeda, S.Morita, M.Hino, T.Oda, J.Kato,
Y.Yamagata, and M.Furusaka, "New Fabrication Method
for an ellipsoidal neutron focusing mirror with a metal
substrate", Optics Express, Vol.22 No.20 DOI:
10.1364/OE.22.024666 (2014)

採択課題番号 26P8-5

中性子ラジオグラフィによる工業製品の内部情報取得とVCAD システムによるシミュレーション（京大・原子炉）齊藤泰司、川端祐司、杉山正明、日野正裕、伊藤大介（理研）山形豊、森田晋也、横田秀夫、世良俊博、加藤純一、池上祐司

39

プロジェクトPR8-5

Evaluation of the Moisture Movement in High-Performance
Concrete Subjected to Heating

M. Kanematsu1, S. Bae1, T. Koyama1, R. Inose1,
N. Tuchiya2, M. Tamura3, Y. Nishio3, T. Noguchi3
D. Ito4 and Y. Saitou4(a)1

Department of Architecture, Tokyo University of Science
Building Research Institute, Material Study Group3
Department of Architecture, The University of Tokyo
4
Research Reactor Institute Kyoto University

2

INTRODUCTION: High-performance concrete (HPC)
has low water-to-binder ratio and it is vulnerable to the fire
exposure, resulting in the explosive spalling of HPC surface at the early stage of fire. The spalling phenomena has
been explained to occur due to the moisture pressure accumulated inside the pore of HPC [1]. However, the actual
mechanism of the spalling has not been fully understood.
To understand the detailed mechanism of spalling in HPC,
2-dimensional moisture movement in HPC subjected toheating was quantitatively assessed in this study.
EXPERIMENTS: The concrete specimen (100×100×20mm3) with water-to-binder ratio of 18 % was prepared.
The initial moisture contents of the specimen was 14.1 %and the heating condition referred to the previous work[2].The TNRF in the B-4 beam-line of neutron flux
1×107n/cm2 was utilized for neutron radiography and thenoise pixel in the images deviating more than 10 grayscalevalues were replaced by the median value of the pixels
around the circle with 2-pixels radius.
RESULTS: Fig.1 presents 2-dimensional distribution ofdifferential moisture contents of paste in the specimen perunit volume. The correlation between the change of watercontent and the intensity of transmitted neutron was examined using specimens with predetermined specific watercontents. As shown in Fig.1, the moisture condensed areas
were observed at the boundary of dried areas, moving up
to the top with the temperature elevation. This phenomenon was also confirmed in our previous work, in the caseof high strength mortar [2]. Furthermore, the presence ofmoisture condensed areas was observed around the coarse
aggregates and the holes created for the internal temperature measurement, which is in good agreement with theprevious numerical model [4]. The interfacial transitionzone around the coarse aggregates is assumed to provide
the space that the condensed moisture can passthrough.The explosive spalling occurred for two times, at
1m26s and 1m27s, respectively. In the area of 0 to 5 mmfrom heating surface, moisture content increase was monitored with the value of 5.0×102 g/cm3 6.0×102 g/cm3 ateach spalling. The influence of vapor pressure induced bymoisture movement on the spalling phenomena of HPC
will be further investigated in the future.
REFERENCES:

(b)

(c)

Fig.1 Two-dimensional distribution of differential moisture contents of paste of HPC per unit volume at (a) 1
min, (b) 4 min, and (c) 8 min after heating[1] T.Z.Harmathy, ASTM, Philadelphia, No.385, 75-95[2] M.kanematsu et al, PJCI, vol36, No.1, 2014[3] J. Zhao, Cem. Concr. Res., 65, 64-75, 2014

採択課題番号26P8-10 高温加熱環境下における高強度コンクリートの水分移動の研究 プロジェクト（東理大・理工）兼松学、Sungchul Bae、小山拓、猪瀬亮（建研・材料）土屋直子（東大・工）田村政道、西尾悠平、野口貴文（京大炉）伊藤大介、齊藤泰司

40

PR8-6

Effect of Gravity on Coolant Distribution in FGHP Heat Spreader

K. Mizuta, Y. Saito 1, D. Ito 1
Faculty of Engineering, Kagoshima University
1
Research Reactor Institute, Kyoto University
INTRODUCTION: Recently, the importance of thermal management in electronic devices has become muchhigher than ever, because the lack in cooling ability insuch devices leads to various reliability problems and low
working efficiency. Particularly, in a light-emitting diode(LED) array, non-uniform temperature distributions
caused by poor heat spreading ability of its substrate ruins the quality of lightning, because the light emitting
efficiency of LED gets lowered with higher working
temperature. To tackle with such problems in thermal
management, vapor chambers would be one of the hopeful candidates as the substrate for its higher effective
thermal conductivity compared with metal heat spreaders[1]. In an ordinary vapor chamber, however, it has beenreported that the heat transfer characteristics are strongly
affected by its installation posture, because the coolant
circulation inside the vapor chamber is strongly affectedby the gravity, which spoils the adoption of vapor chambers for the LED substrate. The authors have been trying
to solve such problems by utilizing a newly developed
vapor chamber called FGHP which is manufactured by
precise etching technique by Molex Kiire Co., Ltd. located in Kagoshima, Japan. In this study, we investigated
the gravitational effects on the coolant distribution in the
FGHP by using neutron radiography at the Kyoto University Research Reactor (KUR).

Fig. 1. Variation of the liquid thickness in the wick areawith input power.
Neutron imaging of the sample was performed at the 1
MW operation mode of the KUR and the exposure timewas 300 s. Neutron images of the sample were utilized to
calculate liquid thickness in the FGHP. The effect ofgravity on the coolant distribution was evaluated by thecalculated liquid thickness in the wick area at different
positions as follows:
1. Vertical position 1 (Top),
2. Vertical position 2 (Bottom),
3. Horizontal position 1 (Left),
4. Horizontal position 2 (Right).
Interrogation window size was 0.41.5 mm2 at each position.

EXPERIMENTS: Experiment was conducted at theE-2 port of the KUR, where the thermal neutron flux atthe sample position was about 3105 cm2s at 5 MW operation. The size of the test sample of FGHP heat spreader
was 65 mm square and 2 mm thick. The test sample wasset vertically, which means that its bottom and top plate
was placed parallel to the gravitational direction. A ceramic heater of 25251.75 mm3 was attached to thecentral part of the bottom plate as a heat source, and the
top plate was cooled by three pin-fin type aluminum heatsinks of 3535 mm2 under natural convection conditions.
K-type thermocouples were utilized to measure both thesurface temperature of the heat spreader and the atmospheric temperature to estimate the thermal resistance of
the FGHP. A CCD camera (BU-53LN, BITRAN Co.
Ltd.) was utilized, which has 4008×2672 pixels and
6
LiFZnS (50 m thickness) was used as a scintillator
screen. The spatial resolution was 9.0 μm/pixel at thepresent system setup, however, the effective spatial resolution was about 50 μm/pixel due to the scintillator
screen characteristics.

採択課題番号 26P8-11

RESULTS: Figure 1 shows the variation of liquid
thickness with heat input. As shown in Fig. 1, the measured values of the liquid thickness in the wick area takethe smallest at the top and the largest at the bottom positions. The measured values range from 200 to 480 m
and increases along with the gravitational direction.
However the liquid thickness remains nearly constantregardless of the heat input. From the design of the inner
structure of the FGHP heat spreader, the maximum liquid
thickness in the wick area can be estimated as 0.6 mm(about 0.1 mm in the middle plates and 0.5 mm in the top
and the bottom plates), therefore, at least 0.1 mm thickliquid layer would be considered to cover the surface ofthe middle plates as the wick structure, which may suggest the surface of the whole wick area does not dry out
even when the FGHP is installed in the vertical posture.
REFERENCES:[1] J. C. Wang, Int. J Heat and Mass Trans., 53 (2010)
3990-4001.

フラットヒートパイプ型ヒートスプレッダ内部における冷媒挙動に関する研究（鹿児島大・工）水田 敬（京大・原子炉）齊藤 泰司、伊藤 大介
41

プロジェクトPR8-7

Study on Visualization of Organic Materials between Metals
for Advance of Industrial Products

K. Hirota1, A. Uritani, K. Watanabe, A. Yamazaki,
D. Sugimoto, Y. Kiyanagi, Y. Shiota, H. M. Shimizu1,
G. Ichikawa1, M. Kitaguchi2, Y. Saito3
Graduate School of Engineering, Nagoya University
Graduate School of Science, Nagoya University
2
Kobayashi-Maskawa Institute, Nagoya University
3
Research Reactor Institute, Kyoto University
1

INTRODUCTION: The machinery industry products
including automobile and aircraft are progressing to highperformance and high precision. One of the desired technique in these development fields of state-of-art technology products is visualization of organic film (oil film
grease, etc.) exist between metals. In the present work we
explore the possibility of observation of the characteristics(shape, nature and the distribution of thickness) of theorganic skin and its dynamic changes.

Fig. 1. Neutron radiography image of the bearings.
Half of these bearings are removed the grease.

EXPERIMENTS:
The measurement was done at E2
beam port in the reactor room. Bearings and an oil pump
are using for the sample materials. The CCD system is
Bitran BU-53LN and the scintillator is 6Li/Zns(Ag) of
thickness 200m, which is prepared RIKEN group andnormally equipped at E2. The neutron (static) radiography image and CT reconstruction images were taken
for both bearings and oil pomp. The CT reconstruction
system is also equipped at E2. The typical exposure timeis one minute for static image in 1 MW mode. This exposure time is decrease to 1/5 at 5MW mode. In the caseof CT measurement, 30 seconds exposure time and 300
images, which are corresponding to 0.6-degree sample
rotation step, are taken.

Fig. 2. CT reconstruction image. Black-and-white
shade is inverted to fig. 1.

RESULTS: Figure 1 shows the neutron radiography
image of bearings. These bearings are all commercial
products. Half of these bearings are removed grease.
White color area means that the neutron beam is easilytransmitted, and black area means absorption. Neutron
beam is expected to be well aborted by grease because ofincluding of hydrogen. Clear grease image were available
to find by comparing the picture between with and without grease. Figure 2 shows the CT reconstruction imageof bearing include grease. Black-and-white shade is inverted to fig. 1. White area indicated the grease in thecase of fig. 2. The grease skin is available to see between
the boll and the frame of the bearing.
We want to observe how to move the grease with bearing rotation as next plan.

採択課題番号 26P8-12

工業製品の高度化に資するためのプロジェクト
金属間有機物の可視化に関する研究（名古屋大・工）瓜谷章、渡辺賢一、山崎淳、杉本大、鬼柳善明、塩田佳徳、（名古屋大・理）
清水裕彦、広田克也、市川豪、（名古屋大・KMI）北口雅暁、（京大・原子炉）齊藤泰司
42

PR8-8Visualization of Flow Inside Fine Scale Wick of Heat Pipe

Y. Tsuji, T. Ito, M. Ogasawara, S. Yanagisawa,
M. Tamaki1, D. Ito2 and Y. Saito2
Graduate School of Engineering, Nagoya University
1
Department of Energy Engineering and Science
Graduate School of Science, Kyoto University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: We study the heat transfer process
on the solid surface covered with liquid water. It is notclearly understand how the heat transfer is enhanced bychanging the condition of solid surface, characteristics ofliquid and flow conditions. We study the heat pipe (Fig.1)
as the simple equipment to study the heat transfer process,and the following points are focused. (1) Character ofsolid surface is changed, such as a water-repellent coat, ahydrophilic coat, and/or a monomolecular film are added
over the solid surface. (2) To change the solid surface
condition as a complicated shape (wick). Such as porous
media is attached on the surface and visualize the boilingprocess inside it. The boiling process is significantly affected by a porous shape and surface condition. (3)Heat
transfer is measured independently, and it is comparedwith boiling process inside the porous media is visualized
by NRG.
The purpose of this study is to enhance the heat transfer
and understand its physical process by analyzing the visualized images by NRG.

Fig.2 Neutron radiography image. (a) air=0ml,(b)air=5ml, (c)air=10ml.
RESULTS: The neutron radio grapy images are shownin Fig.2. We hope to observe the air, vapor and waterphases inside the heat pipe, however it was difficult todistinguish them clearly. The water phase (black) is suppressed in (c) compared with (a) condition. This may be
due to the increase of vapor pressure by adding the air. As
the heat pipe is slightly tilted along the side wall, we canobserve the thin liquid film flowing from top to down.
This is caused by the liquid (water) condensed at the upper region and return to the bottom. On the left-side wall,the liquid film is thicker than that of right wall.
For the qualitative analysis from the digitized image
intensity, the effect of aluminum wall is removed. We
visualized the heat pipe, which does not contain theworking fluid. By using this calibration image, background image is subtracted, that is usually adopted as
NRG procedure. Figure 3 shows the averaged intensity
profiles along the vertical direction of heat pipe. The intensity corresponds to the ratio of water averaged overthe cross direction. The different colors show the conditions (a), (b), and (c), respectively. At the bottom region
close to heater, the intensity of (a) shows the smaller value than other conditions. This indicates the water region
remains much more in (a) condition. However, we can
not distinguish the vapor and air regions. For the final
purpose of our research, the vapor region should be distinguished from other states (water and air phases). The
present techniques are revised in the next stage.

EXPERIMENTS: House-made heat pipe is operated
with supplying the heat by the Peltier module. We change
the conditions of heat transfer with monitoring the NRG
image. The heat pipe is made of aluminum, whose dimension is 20×110×110mm. Heater power is varied
from 6 W to 30W, and the temperature of heater sectionchanges from 40℃ to 70℃. The maximum inside pressure is 36 kPa.
In this measurement, we have to check the basic performance of NRG technique for observing the air, vapor
and water states and their motions. Working fluid is water(20ml), and three different amounts of air (0, 5, 10ml) aresupplied inside the heat pipe. The E2 beam port was used
for NRG experiments.

Fig.3 NRG intensity profiles along the heat pipe.

Fig.1 Schematic view of experimental setup

採択課題番号 26P8-13
微細ウイック内流動のＮＲＧによる可視化に関する研究（名大院工）辻義之、伊藤高啓、小笠原克、玉置昌義（京大・原子炉）齊藤泰司
43

プロジェクトPR10

Project Research on the Elucidation of Generating Mechanism ofDamaged Protein Induced by Aging and Irradiation

N. Fujii

ARS-2: Saito et al. revealed that carotenoids have noeffect on the initial rapid peroxidation during the processof damage to lipid induced by gamma irradiation, but an
optimum concentration of carotenoids inhibits the subsequent oxidative degradation involving radical reactions
during this process.

Research Reactor Institute, Kyoto University
Objectives and Allotted Research Subjects:
The aim of this project research is to elucidate the correlation between the change of the protein structure induced by various post-translational modifications with
UV irradiation, gamma-irradiation, aging and proteinfunction. We also investigate the repair mechanism forthe damaged protein by irradiation. This research program has started in 2013. In this year, the 6 research subjects were carried out. The allotted research subjects(ARS) are as follows;
ARS-1: Detection of D-aspartyl endopeptidases activity
in floral tissues of broccoli (Brassica oleracea var. Italica). (T. Kinouchi and N. Fujii)
ARS-2: Damage to biological molecules induced byionizing irradiation and biological defense mechanisms
against ionizing radiation I. (T. Saito and N. Fujii)
ARS-3: Analysis of aspartate isomerization using protein L-isoaspartyl methyltransferase (PIMT) (Y. Sadakane
and N. Fujii)
ARS-4: Analysis of imbalance in mice exposed toenvironmental stress. (N. Ohgami and N. Fujii)
ARS-5: Identification of biologically uncommon
β-aspratyl residues in proteins using LC-MS/MS (N. Fujii,
S. Kishimoto and N. Fujii)
ARS-6: Sidechain conformers of aspartyl isomersin
crystallin mimic peptide(K. Aki, E. Okamura)
ARS-7: Rapid survey of Asp isomers in disease-related
proteins by LC-MS/MS combined with Commercial
Enzymes (H. Maeda, T. Takata, N. Fujii H.Sakaue, H.
Sasaki and N. Fujii)

ARS-3: Sadakane et al prepared a repair enzyme for aged
proteins, protein L-isoaspartyl methyltransferase (PIMT)
by E. coli expression system, and analyzed the effect of
substrate size on the activity of PIMT. PIMT activity isaffected by length of peptides and the activity is weakerin the shorter peptide. However, the peptides which consist of 5 to 9 amino acids are good substrates for PIMT
regardless the position of L-isoAsp. The feature is usefulto analyze various types of peptide because the shorter
peptides are easily prepared.
ARS-4: Ohgami et al. showed that exposure of mice to
low frequency noise (LFN) at moderate levels causes
imbalance and tried to detect protein aggregation in vestibule of inner ears. Our results suggest that incidence ofprotein aggregation was undetectably low at least in the
exposure condition to moderate LFN.
ARS-5: Fujii et al. established a new method to identify
the β-Asp containing peptides by the analysis of the 2nd
generation product ion spectrum of liquid chromatography - tandem mass spectrometry (LC-MS/MS).
ARS-6: Aki et al. investigated populations of side chain
conformers of Asp isomers (L-α-, D-α-, D-β-Asp) in αAcrystallin mimic peptides by using solution NMR. As aresult, trans conformer was preferredin D-β-Asp,
whereas gauche conformer was abundant in L-α- andD-α-Asp. Trans is thought to be disadvantageous to Asp
isomerization. Therefore, the D-β-Asp is thought to be
the most stable in the 3 isomers.

Main Results and Contents of This Project
ARS-1: Kinouchi et al. detected high D-aspartyl endopeptidase (DAEP) activity in the floret of fresh broccoli(Brassica oleracea var. Italica). DAEP is commonly distributed in animals, and their testes and ovaries are especially shown to have the high DAEP activity. Broccoli
floret is a cluster of numerous small flowers and also
encloses the reproductive organs. Since DAEP activity inother parts of plants, such as stems, leaves and roots,
was not detectable or quite low, it was suggested that thephysiological function of DAEP would contribute to theearly development.

採択課題番号 26P10

ARS-7: Fujii et al. demonstrated a new method for rap-

放射線照射や加齢による蛋白質損傷の化学的解明（京大原子炉）藤井紀子

44

プロジェクトPR10-1

Detection of D-Aspartyl Endopeptidases Activity in Floral Tissues of Broccoli(Brassica oleracea var. Italica)
DAEP was measured at λex = 380 nm and λem = 460
nm.

T. Kinouchi and N. Fujii
Research Reactor Institute, Kyoto University

RESULTS & DISCUSSION: As described in this lastreport, radish taproots were shown to have the DAEP
activity but in quite low amounts [4]. And in tomato
fruits, the DAEP activity was not detectable because endogenous pigments in the extract of tomato fruits would
disturb the measurement. Although the supernatant
extracted from broccoli floret also had a high amount of
the green pigment, the DAEP activity showed 15 times
higher than in radish taproots.
In this report, four broccoli florets were used for the
DAEP assay, and each measured value of the specificactivity was not stable (~±20%). Since each broccoli waspurchased on different day, the different storage periodsof those broccoli florets may have affected the postharvest senescence. Therefore we would like to make thenext issue to observe chronological changes of the DAEP
activity in plant embryo.

D-isomer of aspartate (D-Asp)
INTRODUCTION:
residue is detected in abnormally folded and aggregatedproteins: i.e., crystalline, prion protein and β-amyloid
protein. Accordingly, it is suggested that the formationof D-Asp in those proteins is responsible for the relateddiseases: cataract, prion disease and Alzheimer’s disease,respectively. The D-aspartyl endopeptidase (DAEP),
which we identified from mammalian liver, stereoselectively degrades its substrate at the internal D-Asp residue,
and seems to physiologically serve as a scavenger against
the noxious D-Asp containing-protein and to maintain thenormal protein turnover [1]-[3]. However, the distribution of DAEP in other living-things was not as clear as inanimals. As a result of searching the distribution of
DAEP in various animals, reproductive organs wereshown to have the high DAEP activity as a common feature. Especially this tendency was evident amongaquatic animals, for example, in African clawed frogs(Xenopus laevis) and Japanese green sea urchins (Hemicentrotus pulcherrimus). The high DAEP activity waspractically detectable in their testes, ovaries and unfertilized eggs.
On the other hand, the existence of DAEP in plants
is ambiguous. Considering the distribution of DAEP in
animals, we searched the DAEP activity in the reproductive organ such as a floral tissue of plants.

Table.

Specific activities of DAEP in various samples.
Samples (tissue)

African clawed frog
(Ovary)Radish (taproot)
Broccoli (floret)

EXPERIMENTS:
Plant Material> Fresh broccoli(Brassica oleracea var. Italica) was purchased from a
local supermarket and the floret was separated. Afterany damaged parts were removed from the floret, theremainder was cut into fine pieces and then homogenizedby Polytron® PT2100 agitator in ice-cold sodium phosphate buffer (pH 7.0). The suspension was filteredthrough a double layer of cheesecloth and centrifuged at
600 xg for 10 min at 4°C. Since the supernatant was crude enzyme mixtures that might include not only DAEP
but also other proteases, the appropriate dose of proteaseinhibitor cocktail for plant cell extracts (purchased from
Sigma-Aldrich, Inc) was added into it.
Measurement of DAEP activity> We developed an assay
system for DAEP activity using the synthetic D-Asp conacid
taining
substrate,
Succinyl-D-Aspartic
α-(4-methyl-coumaryl-7-amide) (Suc-D-Asp-MCA) [1].
Supernatant of the above biological materials was mixed
and incubated with 0.1 mM Suc-D-Asp-MCA and theassay buffer (10 mM Tris-HCl (pH 8.5), 200 mM NaCl, 3
The fluorescence of amimM MgCl2) at 25°C.
nomethylcoumarin liberated from Suc-D-Asp-MCA bySpecific activity(% of max in frog)
100
~1.5
~30

REFERENCES:[1] T. Kinouchi et al., Biochem. Biophys. Res. Commun.,
314 (2004) 730-736.
[2] T. Kinouchi et al., Chem. Biodivers., 7 (2010)
1403-1407.
[3] T. Kinouchi et al., J. Chromat. B., 879 (2011)3349-3352.
[4] T. Kinouchi and N. Fujii, KURRI Prog. Rep. 2013(2014) 110.

	
 採択課題番号 26P10-1

D-アスパラギン酸含有蛋白質に特異的な分解酵素の進化生物学的研究	
 	 	
 （京大・原子炉）木野内忠稔、藤井紀子	
 45

プロジェクトPR10-2

Damage to Biological Moleculed Induced by Ionizing Irradiation and
Biological Defense Mechanisms against Ionizing Radiation I
min, and absorption at 535 nm was measured. The
amount of malondialdehyde (MDA) formed was calculated using the molar absorption coefficient (ε) of thecolor substance formed by the reaction (i.e., 1.56 × 105 at
535 nm). Thus, the level of oxidative degradation of
α-linolenic acid was evaluated by measuring the amountof MDA. Analysis of Peroxidation of α-Linolenic Acid:
The method described by Kennedy and Liebler was usedwith some modifications [3]. The gamma-irradiatedsamples were diluted 600-fold with n-hexane, and then
5.0 mL of this solution was evaporated under reducedpressure. The resulting residue was dissolved in 5.0 mLof n-hexane, and the average absorbance of this solution
in the 230–236 nm range, which was derived from theconjugated diene formed, was measured. In this study,
the level of peroxidation of α-linolenic acid was evaluated by determining the relative amount of conjugateddiene formed.
-3
RESULTS: The analyses revealed that 8.5 × 10 M
β-carotene and 5.0 × 10-4 M astaxanthin inhibited
gamma radiation-induced oxidative degradation of
α-linolenic acid; in contrast, 5.0 × 10-5 and 5.0 × 10-6M β-carotene, and 5.0 × 10-7 and 5.0 × 10-8 M
astaxanthin promoted its degradation. On the other
hand, β-carotene and astaxanthin did not affect gamma
radiation-induced peroxidation of α-linolenic acid.
These facts indicated that carotenoids have no effecton the rapid initial peroxidation during the process ofdamage to lipid induced by gamma irradiation, but an
optimum concentration of carotenoids inhibits thesubsequent oxidative degradation during this process.
The present study suggests that radioresistant bacteria
possess the biological defense mechanism involving
the scavenging of ionizing radiation-induced radicals
in lipid regions, such as cell membranes, by red carotenoid pigments, thereby protecting biological lipids
and other biomolecules in the vicinity of the carotenoid against damage induced by radical reactions.

Takeshi Saito and Noriko Fujii
Research Reactor Institute, Kyoto University
INTRODUCTION: Some bacteria exhibit extreme
resistance to ionizing radiation [1]. A common feature ofthese bacteria is that they contain red carotenoid pigments [1]. Colorless mutants of these radioresistant bacteria are more sensitive to gamma irradiation than wild
types [1]. Therefore, carotenoids are thought to be involved in the bacterial defense mechanisms against ionizing radiation [1]. Biological effects induced by
low-linear energy transfer ionizing radiation are mainly
attributed to radicals generated by radiolysis. Carotenoids
have high radical scavenging activity, and they are localized in cell surface lipids in prokaryotes. These facts indicate that carotenoids are likely to defend the cell surface lipids of radioresistant bacteria against ionizing radiation.
When considering the biological defense mechanismof these radioresistant bacteria against ionizing radiation,
it is important to elucidate the effects of carotenoids ondamage to biological molecules, especially biologicallipids. In this study, we analyzed the effect of two typicalcarotenoids, β-carotene and astaxanthin, on the oxidative
degradation as well as peroxidation of biological lipids,
α-linolenic acid, induced by gamma irradiation.
EXPERIMENTS: Sample Preparation: α-Linolenicacid was dissolved in benzene at a final concentration of
5.0 × 10-1 M, and β-carotene and astaxanthin were added
at a final concentration of 5.0 × 10-6 to 5.8 × 10-3 M and
5.0 × 10-8 to 5.0 × 10-4 M, respectively. Gamma Irradiation: The prepared solutions were irradiated with 60Co
gamma rays at a dose of 30 kGy and a dose rate of 400
Gy/min. Analysis of Oxidative Degradation of
α-Linolenic Acid: The method described by Buege andAust was used with some modifications [2].
TCA-TBA-BHT-HCl regent (15% trichloroacetic acid,
0.375% thiobarbituric acid, 0.04% butylated hydroxytoluene, and 0.25N hydrochloric acid) was prepared. The
gamma irradiated sample was diluted 50-fold with benzene. The diluted solution (3.0 mL) was evaporated
under reduced pressure. The resulting residue was dispersed in 9.0 mL of PBS(−) with a sonicator. The dispersed solution (1.0 mL) was combined with 2.0 mL of
TCA-TBA-BHT-HCl regent and thoroughly mixed. The
mixed solution was heated in a boiling water bath for 15

REFERENCES:[1] T. Saito, Viva Origino, 30 (2007) 85–92.
[2] J. A. Buege and S. D. Aust, Meth. Enzymol., 52,(1978) 302-310.
[3] T.A. Kennedy and D.C. Liebler, J. Biol. Chem. 267,
(1992) 4658–4663.

採択課題番号26P10- 2 	
 放射線照射による生体分子損傷と放射線に対する生体防御機構 	
 プロジェクト（京大・原子炉）齊藤	  毅、藤井	
  紀子	
 

46

	
 

PR10-3

Analysis of Aspartate Isomerization Using
Protein L-Isoaspartyl Methyltransferase (PIMT)
Analysis of Aspartate Isomerization Using Protein L-Isoaspartyl Methyltransferase (PIMT)

Y. Sadakane1, N. Fujii2

L-isoAsp were incubated in recombinant PIMT withco-substrate S-adenosyl methionine and the production

1

Department of Pharmaceutical Sciences, Suzuka University of Medical Science2
Research Reactor Institute, Kyoto Universityof SAH was analyzed by reversed-phased HPLC with
4 % acetonitrile solving in pH 4.6 acetate buffer (Fig. 2) .

A)INTRODUCTION: The stereoconversion of aspartyl(Asp) residue arise through intramolecular rearrangement,such as via a succinimide intermediate. L-isoaspartyl
methyltransferase (PIMT) catalyzes repair of L-isoAsp
peptide bonds in aged proteins by transferring a methylgroup from S-adenosylmethionine to a α-carboxyl groupof L-isoAsp residue (Fig.1).


O

H
N
H

OH
H
N

O

R

N
H





O

O

H N

H
R

N
H

O

H
N
H

H
N
H

O



N
H





SAHμM/min

B)

 

CH3

O

H

R



N
H
OH

O

O

0.2#

SAH

H N

R

0.3#

O

O
OH
H
N

0.5#
0.4#

0#

R

R
N
H
O

0.6#

0.1#

 

O

O

0.7#

IQ
TG
TV LD
LD AT
S
HF GISSP E
E
LL DLTADLL SLYAD #LL ALYAD #VY LLY
PD #
VY LA
PD Y#
VY AAY
PD #
SA
LS Y#
DS
Y#



0.8#

N
H

R
N
H
OH

O

05#######################1015#Reten)on#Timemin 

Fig. 1 The β–linkage isomerization and stereoinversion
to D-form of aspartyl residue and PIMT repair system.

Fig 2 Effect of substrate length on the PIMT activity (A)and the determination of PIMT activity by HPLC (B).
Various lengths of peptide were incubated with PIMT
and the generation rates of S-adenosyl homocysteine(SAH) were determined by HPLC analysis.

In this study, we prepared PIMT by E. coli expression
system, and analyzed the effect of various length of substrate on the activity of PIMT.
EXPERIMENTS: The recombinant PIMT protein was
prepared by His-tag conjugated E. coli expression system,and the various lengths of peptide fragments were synthesized by using Fmoc amino acids. To be the substratefor PIMT, L-isoAsp was substituted for the aspartate residues in these peptides. The PIMT activity was measuredby HPLC analysis of S-adenosyl homocysteine (SAH),
which was demetylated product of co-substrate
S-adenosyl methionine for PIMT.

The HPLC profile (Fig 2B) ensures quantitative analysis
of SAH. Fig 2A shows that PIMT activity is affected bylength of peptides and the activity is weaker in the shorter
substrate. However, the peptides which consist of 9 to 5
amino acids are good substrates for PIMT regardless the
position of L-isoAsp. Our recombinant PIMT is able torepair the L-isoAsp residue in the short peptide that consists of five amino acids. The feature is useful to analyze
various types of peptide because the shorter peptides areeasily prepared.

RESULTS: The various lengths of peptide bearing

採択課題番号 26P10-3	  	  	  タンパク質中のアスパラギンおよび	
  	
  	
 	
 	
 	
 	
 	
 	
 	
 	
 	
  	
  プロジェクト	
 
	
  	
  	
  	
  	
  	
  	
  	
  アスパラギン酸残基の異性化と機能変化に関する研究	
 （鈴鹿医療大・薬）定金	  豊	 （京大・原子炉）	
  藤井	
  紀子	
 
47

PR10-4

Analysis of Imbalance in Mice Exposed to Environmental Stress

Nobutaka Ohgami1,2 and Noriko Fujii3
1(ICR) at 6 weeks of age were used for exposure experiments. All experiments were authorized by theInstitutional Animal Care and Use Committee in Nagoya University (approval number: 27241) and Chubu
University (approval number: 2610016) and followed
the Japanese Government Regulations for Animal Experiments. Mice were continuously exposed for 1
month to LFN as previously reported [5]. In order tomorphologically detect protein aggregation, thioflavin-S staining was performed as previously reported[6].

Department of Occupational and Environmental

Health, Nagoya University Graduate School of Medicine and 2Nutritional Health Science Research Center,
Chubu University
3

Research Reactor Institute, Kyoto University

INTRODUCTION: Exposure to noise generated in
occupational and daily environments is one of the risk
factors threating our health [1,2]. Although noise contains sound with broad frequencies, there is very limited information about the frequency-dependent influence of noise on health. Low frequency noise (LFN) is
generated from industrial devices and home electricalappliances at all times. Thus, we are exposed to LFN
generated from various devices on a daily basis. LFN
is defined as noise having the frequency range below
100 Hz [3]. On the other hand, inner ears contain thevestibule as well as the organ of Corti. Vestibular haircells covered with otoconia to sense gravity stimulus.
Impairments of vestibular hair cells have been shownto cause imbalance [4]. Meanwhile, excessive exposure to noise at 1-20 kHz which is audible sound formice and humans has been shown to induce damage ofhair cells with enhanced oxidative stress in the organof Corti in the inner ear in mice. Also, increased oxidative stress has been shown to cause aggregation ofproteins in central nervous system. At present, however, most of the previous studies used broadband noisewith no consideration of specific frequencies. Our previous study has shown that chronic exposure to LFN at
moderate levels causes imbalance involving morphological impairments of the vestibule with enhanced
levels of oxidative stress and positive signals stainedby anti-D-beta-Asp antibody. However, there is limited information about whether exposure to LFN cancause protein aggregation in vestibular hair cells. In
this study, therefore, we exposed mice to LFN (100Hz) for exposure of mice to noise in order to detect theprotein aggregation in vestibules caused by LFN
stress.

EXPERIMENTS:

RESULTS: After exposure for one month to LFN,
behavior analyses including rotarod, beam-crossing
and footprint analysis showed impaired balance in
LFN-exposed mice but not in non-exposed mice. In
contrast, thioflavin-S staining of vestibule in inner ears
did not show positive signals in exposed mice at leastin this exposure condition. Immunohistochemistrywith anti-alpha-synuclein also did not show typical
pattern of the aggregation. Our results suggest thatincidence of protein aggregation was undetectably low
at least in this exposure condition to moderate LFN.
At present, output level of LFN is limited in our LFN
generator system. Therefore, we will renew the generator system to output LFN at larger level. Also, wewill set up an organ culture system of inner ears to
directly expose to LFN. Sensitivity of thioflavin-S
staining is affected by fixation conditions once in awhile. Further study is needed to improve the detection system of protein aggregation in inner ears.

REFERENCES:[1] J.D. Dougherty, O.L. Welsh N Engl J Med (1966)
275, 759-765.
[2] M. Wallenius J Environ Psych (2004) 24, 167–177.
[3] G. Leventhall (2003) A Review of Published Research on Low Frequency Noise and its Effects, Department of Environment, Food, and Rural Affairs(DEFRA), United Kingdom.
[4] X. Zhao et al., Neuroscience (2008) 153, 289-299.
[5] H. Tamura, N. Ohgami et al., PLoS ONE, (2012) 7(6),e39807[6] A. Sun et al., J. Histochem. Cytochem., (2002) 50,
463-472.

Randomly bred wild-type mice	 採択課題番号 26P10-4 騒音ストレスによる内耳タンパク質中のアスパラギン酸残基の異性化の解析	
 プロジェクト	 （名古屋大学）大神信孝（京大・原子炉）藤井紀子	
 48

PR10-5 Identification of Biologically Uncommon β-aspratyl Residues in Proteins Using MS
N. Fujii, S. Kishimoto1 and N. Fujii2

αAT18 peptide (Fig 1a, c), while these product ions were
not observed for α-Asp containing αAT18 peptide (Fig 1b,d). In addition, the y8-91 and y8-73 were also observed in
the 2nd generation product ion spectrum of β-Asp containing αBT4 peptide (Fig 2a, c) but not for α-Asp containing αBT4 peptide (Fig 2b, d). These results clearly
indicated that the y(l-n+1)-91 and y(l-n+1)-73 ions (“l” and“n” represent the length of the peptide and the position of
the Asp residue) of the 2nd generation product ion of thepeptides distinguish the β-Asp containing peptide fromthe α-Asp containing peptide.

Radioisotop Research Center, Teikyo University
1
Faculty of Pharma Sciences, Teikyo University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: We recently developed a new
method for determining peptides containing Asp isomers
at individual sites and for detecting inverted Asp residues
in any protein by using a liquid chromatography - tandem
mass spectrometry system [1]. In order to determine
which types of Asp isomer are present, however, standard
peptides containing Lα, Lβ, Dα, Dβ isomers must be synthesized and their retention times on LC-MS must becompared with those of the sample peptides. The synthesis of the standard peptide contain 4 different Asp isomers per one peptide is time-consuming. Hence, we developed an advanced method for rapidly identifying the
Asp isomers by detecting the specific 2nd generation
product ions for the β-Asp containing peptides using an
ion trap mass spectrometer (ion trap MS).

CONCLUSION: Identification of biologically uncommon β-Asp containing peptide has been established by
the analysis of the 2nd generation product ion spectrumof ion trap MS.

EXPERIMENTS: The peptides containing four different
Asp isomers were made using a Fmoc solid-phase chemistry. The synthetic peptides were human αA-crystallin
sequence from residues 146 to 157 peptides (αAT18 peptide) containing four different Asp isomers;
IQTGLD(Lα-Asp)ATHAER(αAT18Lα-Asp),IQTGLD(Lβ-Asp)ATHAER(αAT18Lβ-Asp),IQTGLD(Dα-Asp)ATHAER(αAT18Dα-Asp),IQTGLD(Dβ-Asp)ATHAER (αAT18 Dβ-Asp) and human
αB-crystallin sequence from residues 57 to 69 peptides(αBT4 peptide) containing four different Asp isomers;
APSWFD(Lα-Asp)TGLSEMR(αBT4Lα-Asp),APSWFD(Lβ-Asp)TGLSEMR(αBT4Lβ-Asp),APSWFD(Dα-Asp)TGLSEMR(αBT4Dα-Asp),APSWFD(Dβ-Asp)TGLSEMR (αB T4 Dβ-Asp).
A mass spectrometry (MS) was performed on an ion
trap system (LCQ Fleet, Thermo). The 1st and 2nd generation precursor ion of αAT18 peptides were selected the[M+2H]2+ ion at 656.3 m/z and the y7 fragment ion at
799.3 m/z. The 1st and 2nd generation precursor ion of
αBT4 peptides was selected the [M+2H]2+ ion at 748.8
m/z and the y8 fragment ion at 908.4 m/z.

Fig. 1. Second generation product ion spectrums of four
isomeric Asp in αAT18 peptide. a) αAT18 Dβ-Asp, b)
αAT18 Dα-Asp, c) αAT18 Lβ-Asp, d) αAT18 Lα-Asp

RESULTS: Fig. 1 shows the 2nd generation product ion
spectrum of αAT18 peptide containing four different Asp
isomers. The specific fragment ions of 726 m/z (y7-73)
and 708 m/z (y7-91) were observed in the spectrum of
αAT18 Dβ-Asp and αAT18 Lβ-Asp. Fig. 2 shows the 2nd
generation product ion spectrum of αBT4 peptide containing four different Asp isomers. The specific fragment
ions of 835 m/z (y8-73) and 817 m/z (y8-91) were observed in the spectrum of αBT4 Dβ-Asp and αBT4Lβ-Asp. The y7-91 and y7-73 were observed in the 2nd
generation product ion spectrum of β-Asp containing

Fig. 2. Second generation product ion spectrums of four
isomeric Asp in αBT4 peptide. a) αBT4 Dβ-Asp, b) αBT4Dα-Asp, c) αBT4 Lβ-Asp, d) αBT4 Lα-Asp

REFERENCES:[1] N. Fujii et al., J. Biol. Chem. 287 (2012) 39992 40002.

採択課題番号 26P10-5 タンパク質中のアスパラギン酸残基の異性体分析方法の開発 プロジェクト（帝京大・中央 RI 教育研究施設）藤井智彦（帝京大・薬）岸本成史（京大・原子炉）藤井紀子
49

PR10-6

Side Chain Conformers of Aspartyl Isomers in Crystallin Mimic Peptide
Here P(T), P(G+), and P(G−) are the probabilities forconformers T, G+, and G−, and J t and J g are the vicinal
spin–spin coupling constants between the α- andβ-protons in the trans and the gauche conformers, respectively[6].

K. Aki., E. Okamura
Faculty of Pharmaceutical Sciences Himeji Dokkyo University
INTRODUCTION: D-β-aspartyl (Asp) residues areaccumulated in aged human-lens αA-crystallin [1] [2].
Natural L-α-Asp isomerize to the uncommon D-β-Asp
form via a succinimide intermediate. D-β-Asp is responsible for the structural change of proteins or peptides,
because D-isomers with different side-chain orientationand β-isomers which prolong main peptide bond can induce uncommon main chain structures, to trigger the abnormal unfolding or aggregation leading to a disease.
Previous studies have suggested that D-β-Asp is morestable than L-α-Asp in human-lens αA-crystallin peptides[3]. However, it remains unsolved why the β-Asp is stable as compared to α-Asp in such peptides.
In this study, the stability between α- and β-Asp forms
in the peptide is discussed in relation to the population ofside-chain conformers (trans (T), gauche+ (G+) andgauche− (G−)) of Asp isomers. By using human-lens
αA-crystallin
fragment,
(T6f:
T55V
CF3-Phe58
65
D SGISEVR ) composed of L-α-, D-α-, and D-β-Asp
58 residues, the vicinal spin–spin coupling constants (J)of Asp 58 Hα-Hβ1 (Jαβ1 ) and Asp 58 Hα-Hβ2 (Jαβ2 )arequantiﬁed and compared by high-resolution solution
NMR to calculate the population of side-chain conformers. Here, the difference in the population of side chain
conformers between L-α-, D-α-, and D-β-Asp is interpreted by how easily the succinimide is formed.

RESULTS: In T6fLα at 37°C, the population of G+ is
39%, the highest in the side-chain conformers of Asp. In
T6fDα at 37°C, the population of G− is the highest(45%), whereas the T conformer is the least (24%). In
contrast, the population of T conformer is most preferable
in T6fDβ at 37°C; more than 50% of the Asp side-chain
is in the T state[4]. Such preferences are the case at all
the temperatures examined. The result shows that the
population of the gauche conformers, G+ and G− is relatively high in α-Asp containing T6fLα and T6fDα, ascompared to the T conformer.
The racemization and isomerization of Asp proceed as:(i) when the carboxylate carbon (C COO−) of the Asp 58
side chain is attacked by the nitrogen (N) of Ser 59, L(orD)-succinimide is formed by the intramolecular cyclization; (ii) L(or D)-succinimide is converted to D (orL)-succinimide through an intermediate that has theprochiral α-carbon in the plane of the ring; and (iii) theD- and L-succinimide are hydrolyzed at either side of
their two carbonyl groups, yielding both α- and β-Asp
residues, respectively [7]. The close distance between
Asp 58 C COO− and Ser 59 N should be advantageous tothis cyclization. For G+ and G− conformers, the distance between Asp C COO− and Ser N is, actually, 3.5 ±0.7 Å, smaller than the distance 4.5 ± 0.5 Å for the T
conformer. Therefore, Asp C COO− in G+ and G− conformers are easily attacked by Ser N for the isomerizationof Asp 58. In contrast, T6fDβ has the highest populationof the T conformer of Asp 58 side-chain. In such case,Ser 59 N in T6fDβ is hard to attack Asp 58 C COO− toform succinimide due to rather long distance between
Asp C COO− and Ser N. Thus, the Dβ form is thought tobe the most stable in the 3 isomers of Asp 58.

EXPERIMENTS:
The isomers of T6f in which
L-α-Asp was replaced with D-α- and D-β-Asp at position
58 were synthesized by using an automated solid-phase
peptide synthesizer (Shimadzu PSSM-8)[4]. Proton-NMR
measurements were carried out on 400 MHz spectrometer(JEOL ECA400) equipped with a super conducting magnet of 9.4 T. A high sensitivity probe (JEOL,
NM40T10A/AT) for 10 mm o.d. sample tube was used.
About 2 mg of T6f peptides was dissolved in 4 ml PBS/D
2O (pD 7.6) and subject to NMR measurement at
10-60 °C. Free-induction decays were accumulated 2048
times. The digital resolution was as high as 0.02 Hz toobtain the coupling constants with high accuracy[4]. The
coupling constants of Asp Hα –Hβ1 (Jαβ1 ) and Hα –Hβ2
(Jαβ2 ) were evaluated by using Asp 58 Hβ at 2.5–2.9 ppm.
Using Jαβ1 and Jαβ2 obtained by the high-resolution 1H
NMR measurement, the population of side-chain conformers of Asp in T6f isomers is calculated by the following equations [5].

REFERENCES:[1]N. Fujii et al., J. Biochem. 116 (1994) 663–669.
[2]N. Fujii et al., J. Biol Chem. 287(NO.47) (2012)
39992-40002,[3]K. Aki et al., PLoS One 8 (2013) e58515[4]K. Aki and E. Okamura Biophys Chem 196 (2015)10-15.
[5]T. Kimura et al., J. Phys Chem B 106 (2002)
12336-12343.
[6] Pachler, K GR Spectrochim Acta 20 (1964) 581-587[7] T. Geiger et al., J. Biol. Chem. 262 (1987) 785–794.

J1  P(T ) J t  P(G  ) J g  P(G  ) J g

J 2  P(T ) J g  P(G  ) J t  P(G  ) J g
P(T )  P(G  )  P(G  )  1

採択課題番号 26P10-6 Asp 異性体含有αクリスタリン部分ペプチドの構造研究（京大・原子炉）藤井紀子
50

プロジェクトPR10-7

Rapid Survey of Asp Isomers in Disease-related Proteins by LC-MS/MS Combinedwith Commercial Enzymes

Hiroki Maeda1, Takumi Takata2, Norihiko Fujii3, Hiroaki
Sakaue4 , Hiroshi Sasaki5 and Noriko Fujii1,2

mers. Similarly, PIMT recognizes only peptides containing Lβ-Asp residues, and paenidase internally cleaves the
C-terminus of Dα-Asp residues.
RESULTS: Figure 1 shows a typical example of theidentification of the Asp 58 isomers in the αA 55-65 peptide (TVLD58SGISEVR, [M+2H]2+ = 588.3) from
αA-crystallin in lens from elderly people. This simplified
approach has been successfully applied to the analysis of
all tryptic peptides in aged lens.
CONCLUSION:This new method is able to search
comprehensively for the Asp isomers in damaged or aged
proteins from all living tissues and cells.

1

Graduate School of Science, Kyoto University
Research Reactor Institute, Kyoto University
3
Teikyo University
4
International University of Health and Welfare
5
Kanazawa Medical University
2

Relative Abundance(%)

Relative Abundance(%)

INTRODUCTION: Until relatively recently, it wasconsidered that D-amino acids were excluded from living
systems except for the cell wall of microorganisms.
However, D -aspartate residues have now been detected
in long-lived proteins from various tissues of elderly humans. Formation of D -aspartate in proteins induces aggregation and loss of function, leading to age-related disorders such as cataracts and Alzheimer disease. A recent
study used a liquid chromatography - tandem mass spectrometry (LC-MS/MS) to analyze isomers of Asp residues in proteins precisely without complex purification of
the proteins. However, to identify the four Asp isomers(Lα, Lβ, Dβ and Dα) on the chromatogram, it was necessary to synthesize reference peptides containing the 4different Asp isomers as standards. Here, we describe amethod for rapidly and comprehensively identifying Asp
isomers in proteins using a combination of LC-MS/MS
and commercial enzymes without synthesizing reference
peptides.
EXPERIMENTS:
Synthesis of peptides containing four different Asp
isomers. The following peptides and their diastereoisomers corresponding to the human αA-crystallin sequence
from residues 55 to 65 (αAT6 peptide) were synthesized
by a Shimadzu PSSM-8 peptide synthesizer. The purityof each peptide was confirmed to be >95% by analytical
RP-HPLC and mass spectrometry.
Preparation of lens proteins. Lens samples (one sampleeach) from elderly individuals (aged 80 years) were homogenized under physiological conditions and fractionated into water-soluble (WS) and water-insoluble (WI)
fractions by centrifugation. The WS protein was dissolved in 50 mM Tris/HCl (pH 7.8), 1 mM CaCl2 buffer
before enzymatic digestion.
Identification of the tryptic peptides and the quantitiontification of the Asp isomers. The protein sample istreated with trypsin, trypsin plus endoprotease Asp-N(Asp-N), trypsin plus L-isoaspartyl methyltransferase(PIMT) or trypsin plus paenidase, and the resulting peptides are applied to LC-MS/MS. Because Asp-N hydrolyzes peptide bonds on the N-terminus of only
Lα-Asp residues, it differentiates between peptides containing Lα-Asp and those containing the other three iso-Fig 1
Identification of Asp
isomers in the WS protein fraction from elderly lens.
(a,b) Peaks in the MS range
588.0-589.5 for αA peptide 55-65
containing Asp isomers before (a)and after 17 hrs of Asp-N treatment (b). (c,d) Peaks in the MS
range 588.0-589.5, showing αA
peptide 55-65 containing Asp
isomers before (c) and after 2 hrs
of PIMT treatment (d). (e,d)
Peaks in the MS range
588.0-589.5, showing αA 55-65
peptide containing Asp isomers
before (e) and after 20 hrs of
paenidase treatment (f). The
asterisked peaks indicate peptide
disappearance.

REFERENCES:[1] N. Fujii, H. Sakaue, H. Sasaki H. and N. Fujii.
J. Biol. Chem. 287, (2012) 39992-40002.
[2] H. Maeda, T. Takata, N. Fujii, H. Sakaue, S. Nirasawa, S. Takahashi, H. Sasaki, Rapid survey of four
Asp isomers in disease-related proteins by LC-MS
combined with commercial enzymes, Anal Chem, 87(2015) 561-568.

採択課題番号 26P10-7放射線、紫外線、加齢による蛋白質中のアミノ酸残基の異性化機構の解明プロジェクト	 （京大・原子炉）高田匠、藤井紀子（京大院・理）前田裕貴	
 (帝京大・ＲＩセ)	
 藤井智彦	
 （国際医療福祉大・薬）坂上	  弘明、（金沢医大・医）佐々木	
  洋	
 

51

PR11 Studies on Actinides and Fission Products Performed at the KURRI Hot Laboratory
T. Fujii

ARS-17 40Ar/39Ar dating of neutron irradiated minerals
and glasses (O. Ishizuka et al).
ARS-18 Radiometric Ar-Ar dating of neutron irradiatedlavas (N. Hirano et al.).

Research Reactor Institute, Kyoto University
1. Objectives and Allotted Research Subjects
Studies on actinide and fission product nuclides withcareful management are being more important for reprocessing, disposal, partitioning, and transmutation processes in the nuclear fuel cycle. Hot laboratory of KURRI is one of core facilities in Japan, in which various
nuclides can be handled. This project enhances utilizationof the KURRI hot laboratory by opening for fundamental
and application studies related to radiochemistry, nuclear
chemistry, environmental chemistry, geochemistry, andso on. Allotted research subjects are;
ARS-1 Complexation of actinides with organic substances (T. Sasaki et al.).
ARS-2 Solubility of actinide compounds in aqueous
media (T. Kobayashi et al.).
ARS-3 Leaching of actinides and FPs from fuel debris(N. Sato et al.).
ARS-4 Neutron irradiation damage of vitrified waste
matrices (T. Nagai et al.).
ARS-5 Ligand exchange reaction of actinides in molten
salts (A. Uehara et al.).
ARS-6 Electrochemical behavior of uranium in pyroreprocessing system (Y. Sakamura et al.).
ARS-7 Structural study of f-elements in molten halides(H. Matsuura et al.).
ARS-8 Molecular dynamics simulation of uranyl ion in
molten salts (N. Ohtori et al.)．
ARS-9 Fundamental study of fission products fortrans-actinide chemistry (Y. Kasamatsu et al.).
ARS-10 Isotope separation by using microreactor (R.
Hazama et al.).
ARS-11 Optical properties of molten aluminum halides(T. Goto et al.).
ARS-12 Precipitation of f-element oxides in molten halides (H. Sekimoto et al.).
ARS-13 Uptake of radiocesium and radiopotassium inplants (T. Ohta et al.).
ARS-14 Quantitative analysis of radionuclides in seawater (T. Kubota et al.).
ARS-15 Isotopic composition of radionuclides in environmental samples (Y. Shibahara et al.).
ARS-16 Noble gas mass spectrometry of neutron irradiated geological samples (H. Sumino et al.).

採択課題番号

2. Main Results and Contents
ARS-1, 2, 3, and 4 were performed in order to deepen theknowledge of nuclear waste management issues. In
ARS-1 and 2, stability constants and solubility productsof actinides were obtained. In ARS-3, leaching kinetics
of actinides and FPs from irradiated Zr alloy was clarified. In ARS-4, a structural change of borosilicate byneutron irradiation was found. ARS-5, 6, 7, and 8 were
performed with the viewpoint of pyroreprocessing. In
ARS-5 and 7, ligand exchange of F- and Cl- for U4+ andNd3+ in molten halides was clarified. In ARS-6, effective
diffusion coefficient of U3+ in porous Zr was determined.
In ARS-8, atomic distances of UO2+ in LiCl melt werecomputed. Polarization of Cl- around UO22+ was found.
ARS-11 and 12 seek applications of molten salt systems
for industrial use, for example, refining. ARS-11 studied
optical properties of molten alkaline chlorides containing
Al. Raman spectra obtained were interpreted by using ab
initio method. ARS-12 focuses on recycling of rare earths.
Solubility of Dy(III) under the coexistence of Dy oxide
and oxychloride in chloride melts was discussed. ARS-10
studied isotope fractionation of Ca. A possible fractionation of 48Ca/40Ca was found. ARS-13, 14, and 15 studied
on redionuclides in soils, plants, seawater, and so on. In
ARS-13, distribution of radiocesium in plants was clarified. ARS-14 presented an effective preparation methodof radiotracers which are useful for environmental science. ARS-15 suggested that precise isotopic analysis of
Cs and Sr is helpful for a rapid source analysis of nuclear
accident. ARS-16, 17, and 18 demonstrated that neutron
irradiation at KUR is usable for the Ar-Ar and I-Xe dating of geological samples.
3. Summaries of the achievements
In this research, by using various unique facilities of
KURRI for actinides and fission products, new and characteristic chemical, kinetic, structural, and thermodynamic data were obtained. These new information encompass solid chemistry, molten salt and solution chemistry, as well as nuclear reactions of f-elements and FPs.
The results are useful either for scientific purpose or fortechnological purpose for nuclear science, environmental
science, geoscience, and general industry.

26P11

ホットラボラトリを活用したアクチニドおよび核分裂生成物元素の化学研究（京大・原子炉）藤井俊行
52

プロジェクトPR11-1

Apparent Formation Constant of Metal Ions with Humic Substances; Modelling

T. Sasaki, T. Kobayashi, T. Koukami, A. Uehara1, T. Fujii1, H. Yamana1, H. Moriyama1

representative values for the intramolecular chelating
effect of the bidentate site fraction. In the case of tetravalent metal ions, the hydrolysis reactions are taken into
account for the analysis of the experimental datasets [3].

Graduate School of Engineering, Kyoto University
1
Research Reactor Institute, Kyoto University

RESULTS:
The present model fairly well reproduced the literatureapparent formation constants of tetravalent Pu/Th (Fig.1),
pentavalent Np, divalent Ca/Co, and trivalent Al/Eu withthe hypothetical humic acid and of tetravalent Th, pentavalent Np, divalent Mg/Ca/Co/Mn/Ni/Cu/Zn/Pb, andtrivalent Eu with the hypothetical fulvic acid under awide range of pH, I, and initial HSs and metal concentration [3]. Some discrepancies between the calculated andexperimental values were recognized and discussed; oneis the I dependence of the values of some metal ions suchas neptunium, and the other is the discrepancy observed
for the system of ultra-trace amount of neptunium, suggesting further effects of not yet identified but muchstronger binding sites in HS. Although the present hypothetical structure is only one example of HS, it provides abasis for further studies of the thermodynamic and kinetic
parameters for complexation reactions.

INTRODUCTION:
A semi-empirical thermodynamic model was developed
to estimate the apparent formation constants of metal ionswith humic substances (HSs), humic and fulvic acids,
over a wide range of solution conditions, i.e., pH, ionicstrength, and HS and metal concentrations.
To understand the fundamental rules of metal complexation with HSs, many researchers have attempted tocharacterize the physical and chemical properties of HSs
in soils, sediments, and natural waters. It has been determined that randomly cross-linked heterogeneous organic
substances generally have similar distributions of a number of specific functional groups, including carboxyl,
phenolic, and alcoholic groups. Towards the ultimate goalof characterizing natural HSs, researchers have proposed
hypothetical HS chemical structures based on results obtained using several analytical methods.
The discrete fragment model has been proposed byour group; it decomposes the organic ligands into discrete
fragments of functional groups and chelating bridges thatconnect the functional groups. The ligand fragments
called as basic ligands were clipped from a “pragmatic”
chemical structure of a humic acid (HA) proposed [1],which were distributed statistically in the HA framework.
The fixed formation constant values of the metal ion witheach ligand was taken from the literature; benzoic acid,
phthalic acid, isophthalic acid, 1,2,3-benzenetricarboxylicacid, 1,2,4-benzenetricarboxylic acid, 2-hydroxybenzoic
acid, phenol, butanedioic acid, and acetic acid. The stericeffect of bidentate binding sites due to the additional stabilization by chelate formation was considered, while theelectrostatic surface potential of the HA molecule in solution was not considered for simplification. The model has
yielded satisfactory results for the apparent complex formation constant of trivalent europium with Aldrich HA
under varied solution conditions, including pH, ionicstrength, and the concentrations of metal ions and HA [2].

Th(OH) - IHSS 1S102H [3]14log βapp

1210
8
6
pH4.7, I=0.1, CM=4E‐9〜6E‐8M
pH4.7, I=0.1, CM=1〜6E‐7M
pH4.9, I=0.01, CM=1〜6E‐8M
pH4.8, I=0.1, CM=1〜6E‐9M

4
2

-8

-6

logCR

-4

-2

Fig.1. Example of comparison between the experimental
apparent formation constants app of Th(IV) with humic
acid (purchased from IHSS) and the simulated curves; CR,molar concentration of HS, CM, initial concentration of
metal ion.
REFERENCES:[1] Schulten, H. R., Schnitzer, M. Naturwissenschaften,
80 (1993) 29–30.
[2] Sasaki, T., Kobayashi, T., Takagi I., Moriyama, H. J.
Nucl. Sci. Technol., 45 (2008) 718–724.
[3] Sasaki, T., Yoshida, H., Aoyama, S., Kobayashi, T.,
Takagi I., Moriyama, H. Radiochimica Acta. (2015) inpress.

THEORETICAL:
The model was modified and applied to several kinds ofmetal ions including actinides, i.e., Th(IV), Pu(IV), and
Np(V), according to following steps; 1) a number of datasets for acid dissociation of various HSs were analyzed
to obtain the representative values for the abundance ratios of the basic ligands and the heterogeneity parameterof HSs, 2) the datasets for complexation of various multivalent metal ions with HSs were analyzed to obtain the

採択課題番号26P11-1
アクチニド元素の水溶液内錯生成反応に関する研究
プロジェクト（京大院・工）佐々木隆之、小林大志、鴻上貴之（京大・原子炉）上原章寛、藤井俊行、山名 元、
森山裕丈
53PR11-2 Temperature Effect on the Solubility and Solid Phase of Tetravalent Metal Hydroxide
T. Kobayashi, T. Sasaki, A. Uehara1, T. Fujii1,
H. Yamana1, H. Moriyama1

indicating the progress of crystallization of initial amorphous hydroxide. The Ksp values after aging at different
temperatures were determined from the analysis of thesolubility dataset in Fig.1. After aging at 60ºC, the solubility was measured at 5, 25, 40 and 60ºC (Fig. 2 ) andthe Ksp at different temperatures. Assuming no temperature dependence of enthalpy change (ΔrHº), the ΔrHº was
calculated for Zr4+ + 4OH– <=> Zr(OH)4 (s,60ºC), whereZr(OH)4 (s,60ºC) represents the solid phase formed at
60ºC. The obtained ΔrHº was slightly higher than theΔrHº (–133.6 kJ/mol) for Zr(OH)4(am) calculated fromthe standard enthalpy of formation [3]. Similar analysis
was performed for the solubility after aging at 5 and 40ºC,
and a trend of ΔrHº for the solid phases formed at different temperatures suggested that the solid phase transformation is endothermic reaction within the investigatedtemperature range.

Graduate School of Engineering, Kyoto University
Research Reactor Institute, Kyoto University

1

INTRODUCTION:
The decay heat emission from vitrified high level radioactive waste in the repository will be transferred to
groundwater aquifers through surrounding engineered
and geological barrier systems. In the early failure scenario of the waste package, long-lived radionuclides including tetravalent actinides (An(IV)) leached in the
groundwater are considered to be exposed to an elevatedtemperature environment up to 100°C [1]. For the safetyassessment of geological disposal, it is required to evaluate a possible impact of elevated temperature on the solubility of An(IV). At 25ºC, the steady-state solubility is
generally controlled by amorphous hydroxide as solubility-limiting solid phase, and described using relevant
thermodynamic constants [1]. However, the amorphoushydroxide was dehydrated and crystalized at elevatedtemperature [2]. Therefore, the thermodynamic estimation of An(IV) solubility needs to clarify the both of hydrolysis constants and solubility product (Ksp) at a given
elevated temperature [3].
In the present study, the apparent solubility of zirconium hydroxide as chemical analogue for An(IV) and the
crystallinity of the solid phase were investigated under
several conditions of temperature (5 to 60ºC). The temperature dependence of solubility product and the enthalpy change were discussed.

-2-2
Zr(OH)4(s)Tmeas = 25°C
Taging[2]
90°C [1]
60°C
40°C
[4]
25°C [2]
5°C

-3

-3
-4

-5

log [Zr]log [Zr]-4

Measurement
Temp. 25ºC

-6

-5
-6

-7

-7

-8

-8

Aging
Temp.60ºC

-9

-9
0

1

2

3

+

4

5

6

-log [H ]EXPERIMENTS:
Sample solutions by oversaturation method were prepared by adding NaOH or HClO4 to the acidic Zr perchlorate solutions ([Zr] = 0.01 mol/dm3 (M)). The ionicstrength (I) was adjusted to be I = 0.5 by adding appropriate amount of NaClO4. After aging the sample solutions in temperature chambers controlled at 5ºC, 40ºC
and 60ºC, the samples were transferred to the thermostat
dry-bath followed by the ultrafiltration and pH measurement at different temperature conditions. After filtrationof supernatants through the ultrafiltration membranes (3kDa – 100 kDa NMWL, Millipore), the apparent solubility of zirconium was determined by ICP-MS. XRD wasused to characterize the crystallinity and the particle sizeof the solid phase.

Taging Tmeas
60°C 60°C
60°C 40°C
60°C 25°C
60°C
5°C

Fig. 1. Solubility ofZr(OH)4(s) after aging atdifferent temperatures.

0

1

2

+

3

4

-log [H ]Fig. 2. Solubility ofZr(OH)4(s) measured at
different temperatures
after aging at 60ºC.

REFERENCES:[1] 2nd progress report on research and development for
the geological disposal of HLW in Japan, JNC Report
TN1410 2000-001, JNC, Tokai, Japan.
[2] Kobayashi T. et al., Radiochim. Acta, 101, (2013)645.
[3] Brown P. et al., Chemical Thermodynamics of Zirconium, Elsevier, North-Holland, Amsterdam (2005).
[4] Sasaki, T. et al., Radiochim. Acta 94, 489 (2006).

RESULTS:
The apparent solubility after aging at 40 and 60ºC andmeasured at 25ºC were lower than those kept at 25ºC,

採択課題番号26P11-2 アクチニド元素および放射性核種の溶解沈殿反応に関する研究 プロジェクト（京大院・工）小林大志、佐々木隆之（京大・原子炉）上原章寛、藤井俊行、山名 元、森山裕丈
54

PR11-3

Research on the Behavior of Actinides and FPs in Fuel Debris
spectrometry were performed using a Ge detector and
Si detector to determine the nuclides leached.
RESULTS:
Figure 1 shows the leaching ratios (R(%)) of
actinides to seawater. There, the clear timedependence cannot be seen in the leaching of
Np, Am and Pu during 31 days leaching test.
Also, their leaching ratios were supressed in
the very low extent (0.02 % or less). The leaching of these actinides are expected to be supressed to very low extent regardless of the oxidation state in the solid phase since the solubilities of both M(III) and M(IV) for Am and Pu,
and Np(IV) are very low at the pH of seawater.
On the other hand, the RU value was about
0.1 % during the leaching test. From this result,
it is considered that the uranium dissolution
from the simulated fuel debris was governed by

N. Sato1, A. Kirishima1, M. Hirano, T. Sasaki2, T.
Kobayashi2, Y. Takeno2, A. Uehira3, T. Fujii3, K.
Takamiya3 and H. Yamana3
1

Institute of Multidisciplinary Research for Advanced
Materials, Tohoku University
2
Graduate School of Engineering, Kyoto University
3
Research Reactor Institute, Kyoto University
INTRODUCTION:

After the LOCA of Fukushima Daiichi NPS, the melted core reacted with coolant at high temperatureforming fuel debris containing fuel and structural materials such as zirconium. Under high temperature
condition in the pressure vessel, several kinds of FPs
and TRU were possibly released into the cooling water
mixed with seawater and the air from the melted coreand its fine debris. Information on the radionuclide
behavior in fuel debris and surface seawater will be
helpful to analyze the forthcoming analysis data about
the contents of minor FPs and TRU in contaminatedwater, and to manage associated secondary wastes.
First, the simulated fuel debris composed of uranium
and zirconium oxides as main constituents was prepared by heat treatment in reductive or oxidative conditions. Then the dissolution behavior of typical gamma-ray fission products and neutron activated nuclides
as well as uranium in solid solutions was investigatedby neutron irradiation and following leaching in the
non-filtrated seawater. Dissolution behavior of MA
was also studied by the used of MA doped simulated
fuel debris.
EXPERIMENTAL:
Three types of UO2-ZrO2 solid solution samples with
Zr concentration of 10, 50 and 90 mol% were preparedby mechanochemical and heat treatments under reductive and oxidative atmosphere. The sample was vacuum-sealed in quartz tube and irradiated for 20 min
using the pneumatic transferring system (Pn-2) at
KUR. For reducing the high radioactivity ofshort-lived nuclides, the sample was left in glove box,
and then suspended in 30 ml of fresh seawater from
Minamisoma city, Fukushima. After the aging time in
the atmospheric condition at R.T., a 10 mL of supernatant was transferred to new sample tube after filtration with 0.45 m (Advantec) or 3 kDa (Microcon,
Millipore) membranes, followed by evaporation of theseawater at 363 K in order to repare a solidified
point-like source. For MA doped sample, similar preparation techniques were applied by using U3O8 powder
with 237Np, 243Am and 236Pu. Gamma- and alpha- ray

the solubility limitation of UO3 2H2O(cr), UO3･
2H2O (am) or maybe their intermediate phaseas discussed in our previous study [1]. These
results suggest that both dissolution andstructure data are essential for fuel debris behaviour. In further study, behavior of actinides
and FP’s from different types of fuel debris will
be discussed.

Figure 1 Time dependence of actinides leaching from thesimulated fuel debris to the Fukushima seawater [2].
REFERENCES:[1] T. Sasaki, Y. Takeno, A. Kirishima, N. Sato, J. Nucl.
Sci. Technol., 52 (2015) 146-150.
[2] A. Kirishima, M. Hirano, T. Sasaki, N. Sato, J. Nucl.
Sci. Technol., in press, doi: 10.1080/00223131.2015.
1017545.

採択課題番号 26P11-3
燃料デブリ中のアクチノイドおよび FP 元素の挙動に関する研究
プロジェクト （東北大多元研）佐藤修彰、桐島 陽、平野正彦（京大院工）佐々木隆之、小林大志、竹野 佑（京大・原子炉）上原章寛、藤井俊行、高宮幸一、山名 元

55PR11-4

Effect on Borosilicate Glass Structure by Neutron Irradiation

T. Nagai, A. Miyauchi, Y. Morikawa, A. Uehara1, and T.
Fujii1

ation, it could be observed that the peak heights of Q4 andQ3 decreased and those of Q2 and Q1 increased after theirradiation, as shown in Fig. 1. These height changes ofQn, n=1-4, suggested the feasibility that a generated Li by
the neutron irradiation disconnects the Si-O bridging
structure in a borosilicate glass. However, this Si-O
bridging structure is direct disconnected by γ ray included in the neutron irradiation and the additional experiments needs for understanding of the irradiation effect.

Japan Atomic Energy Agency (JAEA)
1
Research Reactor Institute, Kyoto University
INTRODUCTION: A high-level radioactive liquid
waste including fission products, FPs, from a reprocessing process for spent nuclear fuels is processed into asolidified waste glass made by using a borosilicate glass
as media. Many studies of the effect on borosilicate glass
structure by irradiation have been carried out by irradiation of α ray, β ray, and γ ray which would be generated
from FPs of the waste glass. However, that effect by aneutron irradiation has not been much evaluated. In thisstudy, the borosilicate glass samples were irradiated byneutrons, and the glass structure change after the irradiation was measured by Raman spectrometry.

1.2

non-irradiation
irradiation for 10 min

normalized intensity

1

EXPERIMENTS: The borosilicate glass samples wereprepared 2 compositions. The raw material reagents of
SiO2, H3BO3, Na2CO3, Li2CO3, and rare earth oxides assimulated FPs were placed in an alumina crucible andwere melted at 1150°C in an electric furnace. After themolten samples were solidified by cooling to room temperature, they were cut into thin plates. In the irradiation,
the glass samples of thin plate were set in a polyethylene
tube and were irradiated under the condition of 1000 kW
for 10 min in the Pn-2 of KUR. After the radioactivity ofthe samples was sufficiently attenuated, the Raman spectra of the glass sample were measured by using a laser
Raman spectrometer, NRS-3100 of JASCO. For the effect on borosilicate glass by the nuclear reaction of
10
B(n,α)7Li, Peuget, et al have evaluated the B-O structure by using NMR measurement and Raman spectrometry[1], our study was examined the Si-O structure.

0.8

Q3
0.6

Q2
0.4

Q4

0.2

Q1
0
1250

1200

1150

1100

1050

1000

Raman shift (cm-1)

950

900

850

(1) 63SiO2-16.6B2O3-19Na2O-1.4RE2O3.
1.2

non-irradiation
irradiation for 10 min

normalized intensity

1

RESULTS: As a structural change of the sample by theirradiation, an amount of Li would be increased by the10
B(n,α)7Li reaction, and Li was expected to disconnect
to the Si-O bridging structure. By evaluating the Raman
shift of the Si-O structure, it was confirmed to be the effect on the borosilicate glass structure by the irradiation.
The Raman shifts of Si-O 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 numberof non-bridging oxygen, NBO, of the Si-O structure.[2] In
this measurement of borosilicate glass, those Raman
shifts were observed in 850-1250 cm-1 and the measured
spectra could be separated into Gaussian waves as shownin Fig. 1. The Raman peak of Q4 structure without NBO
appeared in 1140-1150 cm-1, and those of Q3, Q2, and Q1
structures with the NBO number = 1, 2, and 3 were in
1070-1090, 1000-1020, and 920-930 cm-1 respectively.
Comparing with the Raman shifts before and after irradi-

0.8

Q2
0.6

Q3
0.4

Q4

0.2

0
1250

Q1

1200

1150

1100

1050

1000

Raman shift (cm-1)

950

900

850

(2) 63SiO2-16.6B2O3-8.1Li2O-10.9Na2O-1.4RE2O3.
Fig. 1. Raman spectra of glass samples and their separated Gaussian waves. Open circles and fine lines
are a non-irradiation sample, and closed circles anddotted lines are after irradiation.
REFERENCES:[1] S. Peuget, et al, Nucl. Inst. Methods in Phys. Res. B,
327 (2014) 22-28.
[2] P. McMillan, Am. Mineralogist, 69 (1984) 622-644.

採択課題番号 26P11-4 中性子照射によるホウケイ酸ガラス構造への影響評価
プロジェクト（原子力機構）永井崇之、守川 洋、宮内厚志（京大・原子炉）藤井俊行、上原章寛
56PR11-5

Ligand Exchange of Uranium (IV) Chloro- and Fluoro- Complexes in High
Temperature Molten NaCl-CsCl Eutectic
analysis data of U4+ in CsCdBr 3 [2] and LiYF 4 [3],absorption bands of the 5f 2-5f 2 transition of U4+ wereassigned as follows; the 1I 6 ← 3H 4 transition at
22500-19000 cm-1, the 3P 1 ← 3H 4 transition at 17800
cm-1, the 1G 4 , 1D 2 , 3P 0 ← 3H 4 transition at
17000-14000 cm-1, the 3H 6 ← 3H 4 transition at
13100-12000 cm-1, the 3F 3 , 3F 4 ← 3H 4 transition at
11100-7500 cm-1, and the 3H 5 ← 3H 4 transition at
6500-5000 cm-1.

A. Uehara1, T. Nagai2, T. Fujii1, H. Moriyama1, and H.
Yamana1
Research Reactor Institute, Kyoto University
Nuclear Fuel Cycle Engineering Lab., Japan Atomic
Energy Agency

1
2

INTRODUCTION:

In the non-aqueous reprocessing process of spent nuclear fuels by the pyrometallurgical and the electrowinning methods, a spent fuel is dissolved into
molten LiCl-KCl or NaCl-CsCl eutectic melt and dissolved uranium and plutonium ions are recovered as
metal or oxide. In the present study, the chemical
property and coordination circumstance of the complexes of U4+ under the coexistence of fluoride ions inmolten NaCl-CsCl eutectic were investigated by absorption spectrum measurements.

molar absorptivity/ M-1cm-1

10

U4+-Cl complex
5

EXPERIMENTAL:

All experiments were carried out under an argon atmosphere, in which humidity and oxygen impurity
were continuously kept less than 1 ppm. The electronic absorption spectra of uranium ions in the melts were
measured by using an UV/Vis/NIR spectrometer(V-570, JASCO Co.). The analytical light from a lightsource (a tungsten halogen lamp and D 2 O lamp) was
guided to the electric furnace with quartz windows byusing optical fibers, and the light passed through thesample in a quartz tube with a 10 mm light path inside
the furnace. The light which traveled through the furnace was again guided to the spectrophotometer, and a
monochromator was set in front of the detectors todecrease the background noise. The light intensity forthe molten alkali chloride (I 0 ) and that including uranium (I) was measured in the wavelength range of 300– 2000 nm at 1 nm intervals. Wavelength was converted to wavenumber in this work. The molar absorptivity was calculated by using –log (I/I 0 ) and total
volume of the solution. All the experiments were performed at 923K ± 3K.

U4+-F complex
0
23000

20000

17000

[F]/[U]
0
0.09
0.17
0.31
0.47
0.89
1.3
1.7
2.6
9.5
17

14000

wavenumber / cm-1

Fig. 1. Molar absorptivity of U4+ depended on the concentration of NaF in molten NaCl-CsCl eutectic at 923K.
Concentration ratios of F- by U4+ (r F ) are 0, 0.09, 0.17,
0.31, 0.47, 0.89, 1.3, 1.7, 2.6, 9.5, and 17.

When 9.36 × 10-3 M NaF was added in the melt, absorption peaks decreased. Molar ratio of fluorine byuranium (r F ) added in the melt was changed from 0.09
to 17 by adding NaF pellet as shown in Fig. 1. Absorption peaks corresponding to 14903, 16501, and 22123
cm-1 decreased with the increase of r F from 0.09 to 1.7
and isosbestic points at 13774, 15772, 16181, 17793,
and 19305 cm-1 were observed. This result means that
two species of complexes composed of U4+, Cl- and Fare equilibrated. However, when r F was over 9.5, another peaks at 15847, 17331, and 19646 cm-1 wereobserved. This indicates that another complex composed of U4+, Cl-, and F- is formed. After 10 hours aging, red color precipitates were found on the bottom of
the cell.
REFERENCES:[1] Nagai, et al., J. Nucl. Sci. Technol., 42,1025-1031 (2005).
[2] Karbowiak, et al., Chem. Phys., 308, 135-145

RESULTS:

Molar absorptivity of absorption spectra of U4+ in thepresence of F- was plotted as a function of wavenumber in Fig. 1. When an absorption spectrum of
0.106 M U4+ in the absence of F- was measured, molar
absorptivities of each peak wavenumber at 14903,
16501 and 22123 cm-1 agreed with the reported values[1]. By comparing these values with the crystal field(2005)[3] Hubert, et al, J. Luminescence, 60&61, 245-249(1994)

採択課題番号 26P11-5
イオン液体中におけるアクチニドイオンの溶存状態研究（京大・原子炉）上原章寛、藤井俊行、森山裕丈、山名 元（原子力機構）永井崇之

57

プロジェクトPR11-6

Evaluation of Parameters Governing Anodic Dissolution of
U-Zr Alloy in Molten LiCl-KCl

M. Iizuka1, Y. Sakamura1,
T. Fujii2, A. Uehara2 and H. Yamana2

or simple multi-diffusion layer model [1]. Then, the series of the electrochemical operations, including the CP
measurement at constant current density and the rest period in open circuit situation between the measurements,
were digitally simulated by discretization of the diffusion
layers around the U-Zr alloy into elements of 10 to 20µm thickness using finite element method. The calculation result indicated that the transition time evaluatedfrom CPs shown in Fig. 2 can be properly reproduced byassuming the effective diffusion coefficient of U(III) in
the porous Zr layer to be 0.6 ~ 0.8×10-5 cm2/s, which isconsistent with the value 0.7×10-5 cm2/s evaluated fromthe analysis of the longer-term electrorefining experiments [1].

1Central Research Institute of Electric Power Industry
Research Reactor Institute, Kyoto University

2

INTRODUCTION: Analyses of the electrorefining
process for the pyrometallurgical reprocessing of metallic
fast reactor fuel using the multi diffusion layer anodemodel [1] have shown that (a) solubility of UCl3 in
LiCl-KCl melt, and (b) the diffusion coefficient of actinide ions in the porous Zr layer formed at the surface ofthe spent metallic fuel by selective dissolution of the actinides, have great influence on major performance, suchas processing rate and separation between the actinides
and Zr. In this study, chronopotentiometry (CP) was applied to evaluation of these important parameters at
U-9wt%Zr alloy anode.

Current density
1.14 A/cm2
0.76 A/cm2

EXPERIMENTS: Modification of CP theory to beadapted to a situation, where the concentration reaches
saturation by a constant current producing the species
electrochemically, has been reported before [2]. Since
diffusion coefficient of U(III) in LiCl-KCl is known [3],solubility of UCl3 in LiCl-KCl was evaluated using thisdata and τ obtained by CP in this study. After formationof a porous Zr layer by selective anodic dissolution of U
from the U-Zr alloy, CP was performed again. In this step,theoretically, the effective diffusion coefficient of UCl3 in
the porous Zr layer can be estimated using its solubility
data which has been just evaluated in the previous step.
The experimental setup and procedure have been also
reported before [4]. All the experiments were carried out
at 773 K, in a high-purity Ar atmosphere glove box in
KURR hot cell laboratory.

0.57 A/cm2

0.38 A/cm2

Transition time τ

773 K
U in LiCl-KCl : 6.81×10-5 mol/cm3

Fig. 1. Chronopotentiograms obtained with U-Zr
alloy before formation of porous Zr layer.
0

U in LiCl-KCl : 6.81×10-5 mol/cm3, 773 K
Current density : 0.57 A/cm2-0.2

Interval between
measurement

D

Potential (V vs.Ag/AgCl)-0.4

RESULTS: The CPs obtained using U-Zr alloy before
the formation of the porous Zr layer are shown in Fig. 1.
The solubility of UCl3 was evaluated to be 0.00449
mol-U/cm3 so that its averaged diffusion coefficient determined from these CPs agrees with the value in literature (1.45 × 10-5 cm2/s) [3]. Subsequently, CPs were
measured after the formation of the porous Zr layer. In
this case, the diffusion coefficient could not be evaluateddirectly from τ value, since the period until diffusion limit of U(III) varied in every measurement even with thesame current density, as shown in Fig. 2. The reason forthis behavior was considered that the decay of UCl3 concentration gradient in the porous Zr layer caused by the
CP measurement requires a long duration due to the expected lower diffusion coefficient and the large thicknessof the layer. Such complicated condition and resulting
behavior in the actual CP measurement cannot be explained using either the basic electrochemical theory [2]A > 5 min >B > 20 min >C > 20 min >D > 45 min >E > 85 min > F

A
C

-0.6

E
B

-0.8

F

-1

-1.2
0

20

40

60

Time (s)Fig. 2. Chronopotentiograms obtained with U-Zr
alloy after formation of porous Zr layer.
REFERENCES:[1] M. Iizuka et al., J. Nucl.Sci.Technol., 47 (2010) 1140.
[2] M. Iizuka et al., KURR annual report 2010.
[3] S. A. Kuznetsov, et al., Electrochim. Acta, 51 (2006)
2463.
[4] M. Iizuka et al., KURR annual report 2005.

採択課題番号 26P11-6 乾式再処理に関するウラン化合物を用いた基礎研究㸦㟁୰◊㸧ᆏᮧၿ἞ࠊ㣤ሯᨻ฼ࠊ㨶ఫᾈ୍ࠊᮧୖẎ㸦ி኱࣭ཎᏊ⅔㸧⸨஭ಇ⾜ࠊୖཎ❶ᐶࠊᒣྡඖ

58

プロジェクトPR11-7 Electrochemistry and Structural Analysis of Cations in Molten Subhalide Systems:
Fluoride Addition Effect on Voltammograms and UV-vis Spectra of Neodymiumcationin Molten Chlorides
H. Matsuura, A. Nezu, H. Akatsuka, A. Uehara1,
H. Yamana1, T. Fujii1sity was assumed to be the additivity of molar volume ofeach component, and refractive index was temporary
used from the value of KCl due to the non-availability ofthe data of CsCl.

Research Laboratory for Nuclear Reactors,
Tokyo Institute of Technology
1
Research Reactor Institute, Kyoto University

RESULTS and DISCUSSION: Figure 1 shows the differential pulsed voltammograms of cathodic sweeps which
exhibit mainly neodymium reduction peaks. On the contrary to previous measurements[1,2], the potential of neodymium reduction to metal was not shifted positively,
however, drastic negative shift depending on fluoride addition did not occur as well. More strikingly, with increasing fluoride amount, the potenital gap between Nd3+/Nd2+
and Nd2+/Nd decreased, thus disproportionation reaction
may be restricted by addition of fluoride. The variation ofoscillator strength of hypersensitive transition absorptionof neodymium at ca. 589 nm depending on fluoride addition has been evaluated. This absorption peak has been
considered to the indication of coordination symmetryaround neodymium cation, i.e. 6 coordinated octahedral
species, and the smaller value relates to more perfectly
symmetric. One striking feature is that with increasing
fluoride amount until ca. F/Nd = 2 in molten
NaCl-CsCl-NaF, the value of oscillator strength once increases until F/Nd = 2, and decreases rapidly. While inmolten LiCl-KCl-LiF, the value of oscillator strength decreases almost linearly.

INTRODUCTION: Neodymium is the one of the rareearth fission products and was used as the prototype ofsome trans uranium elements due to its similarity of electrochemical behavior. Also, neodymium is one of important materials since it has been widely utilized at magnets
in the motors, and effective recycling technology fromthe end products has been waiting for a long time. Although molten salt should be relatively constructed by asimple structural model due to the predominant ionicspecies in liquid phase, electrochemical behavior has notbeen well understood by the microscopic point of view.
For a recent few years, the electrochemical behavior ofrare earths including neodymium in the molten chlorides
with small amount of fluorides has been focused, andstructural elucidation by extended absorption fine structure and UV-vis spectroscopy of neodymium in molten
salts has been performed [1,2]. In this year, fluoride concentration dependence on the voltammograms of neodymium in molten LiCl-KCl and spectra of neodymium
in molten NaCl-2CsCl was remeasured and the structuralvariation is discussed newly by some parameters derived
from the Judd-Ofelt analysis.

0

EXPERIMENTS: All the electrochemical experiments
using molten salts have been performed in an electric
furnace which is built inside a glove box filled with anargon atmosphere in high purity using an electrochemical
analyzer. Cyclic voltammetry, differential pulsed voltammetry and linear sweep voltammetry have been performed by using the electrodes as follows: working electrode: tungsten, counter electrode: pyrocarbon and reference electrode: silver wire dipped in molten LiCl-KCl
eutectic + AgCl (1 mol%) inside the borosilicate tube,
respectively. Silica glass tube was used as a crucible. To
observe the fluoride addition effect, 0 to 20 times amountof LiF to the concentration of neodymium was added tothe molten salt. All measurements have been performed
at 773 K. UV-vis spectroscopy of neodymium in molten
NaCl-CsCl-NaF at 953 K has been carried out by using
the spectrophotometer. A quartz cell with 10 mm of lightpath was used for the molten salt container, and experimental procedure was exactly the same as that describedin the report of the last year. For the calculation of oscillator strength of the hypersensitive transition and derivation of 2,4,6 parameters by the Judd-Ofelt analysis, den-

x0LiF
x1LiF
x2LiF
x3LiF
x4LiF
x5LiF
x6LiF
x8LiF
x10LiF
x12LiF
x15LiF
x20LiF i [cm-2 A]

-0.5

-1

-1.5

-3

-2.5

-2

-1.5
-

E [V] vs. Cl 2 / Cl

Fig. 1 Differential pulsed voltammograms of cathodic
sweeps of neodymium in molten LiCl-KCl-LiF.
REFERENCES:[1] Y. Shimohara et al, Molten salt chemistry and technology, John Wiley & Sons (2014) 577.
[2] K. Fujita et al, Proc. AMS4, (2012) 264.

採択課題番号 26P11-7

アクチニド元素及び FP 元素含有ハロゲン化物の XAFS 構造解析 プロジェクト
および可視紫外分光研究（東工大・原子炉研）松浦治明、根津 篤、赤塚 洋 （京大・原子炉）上原章寛、山名 元、
藤井俊行
59Polarization Effect of Chloride Ions on Uranyl Ion in Molten LiCl

PR11-8

N. Ohtori, Y. Ishii, A. Uehara1, T. Fujii1, H. Yamana1
Department of Chemistry, Niigata University
Research Reactor Institute, Kyoto University

10

INTRODUCTION: Molten salts are promising solvents for actinides in reprocessing of nuclear fuel. However, knowledge of chemical stability of ionic species inmelts is still inadequate to maximize their potential abilities. Information on local structure around ionic species
in melts may provide useful measures for their stability inmelts. Molecular dynamics (MD) simulation is a powerful tool to elucidate such structures microscopically. In
particular, recent MD simulations with polarizable ionicmodel (PIM)[1,2] have brought much progress in understanding of structure in ionic melts: they have successfully revealed more reliable picture of local structure in
UCl3[2] which is comparable with those from XRD study.
In this work, we have performed MD calculations ofmolten LiCl containing uranyl ion using PIM for chloride
ions, and investigated the effect of polarization of Cl- ionson local structures around uranyl ion.

8

1

g(r)

6

0
1.5

RIM

U=O

1.77 Å

1.80 Å

1.78 Å

1.77 Å

U-Cl

2.73 Å

2.64-2.71 Å

2.78 Å

2.94 Å

2.5

3.0

3.5

4.0

4.5

5.0

5.5

6.0

Fig.1 Radial distribution functions for U and Cl pairobtained from the present calculations.

g(r)

2

1

: CPMD
: PIM
: RIM

0
2

3

4

5

6

7

8

9

10

11

r/Å
Fig.2 Radial distribution functions for U and Li pairobtained from the present calculations.

REFERENCES:[1] P. A. Madden, R. Heaton, A. Aguado and S. Jahn, J.
Mol. Struct.:THEOCHEM, 771 (2006) 9-18.
[2] Y. Okamoto, P. A. Madden and K. Minato, J. Nucl.
Mater. 344 (2005) 109-114.
[3] http://www.cpmd.org/

Table 1 Intraionic distance between U and O in uranyl
ion and interionic distance between U and Cl in molten
LiCl containing uranyl ion
PIM

2.0

r/Å

RESULTS: Figures 1 and 2 show radial distributionfunctions for U and Cl pair and U and Li pair, respectively, obtained from the present calculations. Table 1 summarizes intraionic distance between U and O in uranyl
ion and interionic distance between U and Cl which arenear neighbors with each other. These results clearlyshow effects of polarization of Cl- ions on the coordination structures around uranyl ion. That is, we have foundthat PIM can reproduce the results by first-principle MD
simulation better than RIM.

CPMD

4
2

CALCULATION: MD calculations have been carried out using PIM for molten LiCl containing UO22+ ion.
The system included 500, 502, and 1 ions for Li+, Cl-, andUO22+, respectively. MD calculation without polarizationof Cl- ions has also performed, which is referred here to
as RIM: rigid ion model. Furthermore, first principle MD
simulation has been performed using the CPMD code[3]for the system with similar composition but smaller size.
The temperature was set at 1073 K in all the calculations.

Expt.

: CPMD: PIM: RIM

採択課題番号 26P11-8
融体中での f-元素の分子動力学計算と実験系の照合研究 プロジェクト（新潟大・理）大鳥範和、石井良樹 （京大・原子炉）上原章寛、藤井俊行、山名 元

60PR11-9

Study of Isotope Separation of Strontium andCalcium via Chemical Exchange Reaction

R. Hazama, Y. Sakuma1, A. Ito, T. Fujii2, S. Fukutani2, Y.
Shibahara2

0.31
(Sr)

Cation-exchange chro- 25±0.2[7]matography with Sr lactate.
100
LLE with DC18C6.
25
[8]
(Ca)
0.07M CHCl3
36-15
LLE
with
10-50
[9]
(Ca)
HDEHP(di(2-ethylhexyl)
orthophospheric acid)130
LLE with amalgam.
25
[10]
(Ca)
0.27-0.68M Ca/liter Hg
2.3
Ion exchange chromaroom
[11]
(Ca)
tography with Dowex50
temp.
98
CRC(cryptand2B.2.2).
20
[12]
(Ca)
0.01M
CaCl2+CH3OH/CHCl363
CRC (18C6)
20
(Ca)
0.01M
CaCl2+CH3OH/CHCl3
2.8
Iminodiacetate resin
25
(Ca)
0.95M
NaCl+0.05M
CaCl2
56-130CRC (cryptand2B.2.2)-21-21[13](Ca)
CH3OH/CHCl3/H2O
24
CRC (benzo-18C6).
30
[14]
(Ca)
0.02M Ca + 9M HCl
76
CRC (benzo-18C6).
40
[15]
(Ca)
9M HCl (0.8mmφ,1m)
8.9
CRC (benzo-15C5).
50(Ca)
12M HCl (0.8mmφ,1m)
150 *LLE with DC18C6
20
This
(Ca)
0.07M CHCl3
work
Table 1. Unit mass enrichment factors of Sr and
Ca isotope separation.*: Preliminary
REFERENCES:[1]Y. Fujii et al., Z. Naturforsch., 44a (1989) 395.
[2] K. Nishizawa et al., J. Nucl. Sci. Technol., 32 (1995)
1230.
[3] R. Hazama et al., Proc. of 6th Rencontres du Vietnam,
Gioi Publishers (2007) 383: arXiv0710.3840.[nucl-ex].
[4] Y. Fujii et al., Isotopes in Environmental and HealthStudies, Vol. 46, No.2, (2010) 233.
[5] Y. Ban et al., Sep. Sci. Technol. 36(2001)2165.
[6] J. Aaltonen, Suom. Kem., B45 (1972) 141.
[7] T. Oi et al., Sep. Sci. Technol., 27 (1992) 631.
[8]B.E. Jepson et al., J. Inorg. Nucl. Chem.38(1976)1175.
[9]E.P. Horwitz et al., J. Chromatography 125(1976)203.
[10]D. Zucker et al., J. Chem. Phys. 41(1964)1678.
[11] B.E. Jepson et al., Sep. Sci. Technol. 19(1984)173.
[12] B.E. Jepson et al., Sep. Sci. Technol. 25(1990)1893.
[13]K.G. Heumann et al., Angew. Chem. Int. Ed. Engl.
19(1980)406.
[14]K. Hayasaka et al., Prog. Nucl. Energ. 50(2008)510.
[15]S. Nemoto et al., J. Nucl. Sci. Tech. Vol. 49, No. 4,(2012) 425.

Graduate School of Human Environment, Osaka Sangyo
University
1
Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology,
2
Research Reactor Institute, Kyoto University
INTRODUCTION: Anomalous mass dependence wasexperimentally observed in uranium isotope fractionation
by Fujii et al., in the late 80’s[1] and Nishizawa et al.,suggested that odd-even staggering may be due to the
nuclear charge density difference in the middle of 90’s[2]for the case of strontium. Calcium is congener of strontium and easy to handle to check the isotope effects[3,4].
EXPERIMENTS: Isotopic enrichment occurs according
to the following chemical exchange reaction:40
Ca2+(aq) +48CaL2+(org)48Ca2+(aq) +40CaL2+(org) (1)where L represents macrocyclic polyether(18-crown-6).
As a result, 40Ca is enriched in the organic-phase (org)crown solution and the heavy isotopes of 48Ca tend toconcentrate in the aqueous (aq) phase. The mass effect isobserved by the thermal ionization mass spectrometer(TIMS) measurement of calcium isotope ratios for themass range from 40-48 atomic mass unit (amu).
RESULTS: Unit mass enrichment factors of Sr and Ca
isotope separation are summarized in Table 1. In general,a crown ether gives a large separation factor with morethan ten times, compared with an ion exchange method
and has an applicable ability of separation in reality.
Method and system
Temp.
Ref.
ε/△M
-5
(℃)
[×10 ]
51-17
(Sr)

14
(Sr)
5.6
(Sr)
2.3
(Sr)

Liquid-liquid extraction(LLE) with dicyclohexano-18-crown-6(DC18C6).
2.3M-0.5M Sr in aqueous phase.
Crown-ether resin chromatography (CRC). 1.3m
0.1-0.01M Sr + 2M HCl
CRC. 1.3m
0.1M Sr + 3M HNO3α-hydroxyisobutyrate

20±0.5

[2]

35±2

[5]

35±2
Not
specified[6]

採択課題番号26P11-10 ストロンチウム及びカルシウムの化学交換法における同位体分別研究 プロジェクト（大産大院・人間環境）硲 隆太、伊藤彩 （東工大・原子炉研）佐久間洋一（京大・原子炉）藤井俊行、福谷哲、芝原雄司
61

PR11-10 Experimental and Calculated Optical Properties of Molten Alumnium Chloride Melts
T. Goto, K. Hachiya1, A. Uehara2, T. Fujii2, H. Yamana2

cally at 1 : 1-ratio with increasing CsCl content. Our calculation seems to reproduce fluctuations in the structural
rearrangement at that mixing ratio.

Graduate School of Science and Engineering, Doshisha
University
1
Graduate School of Energy Science, Kyoto University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: Molten AlCl3 and ACl-AlCl3 (A:alkaline metals) have been attractive targets of studies
from both fundamental and application viewpoints, because of their relatively low melting points which lead totheir eﬀectiveness. The structure of the melts contains avariety of coordinations which have long been investigated and mainly consists of covalent bonding between
Al-Cl. In this study, Raman scattering measurements are
performed to investigate into their bonding structures,and the spectra are analyzed with ab initio simulations.
We focus our study on CsCl-AlCl3 binary and
LiCl-KCl-CsCl-AlCl3 ternary systems
EXPERIMENTS: Raman scattering spectra obtained
in KURRI were simulated by calculations with GAUSSIAN09 simulation package. Up to 2 ps trajectories of ionsin the melts were calculated with a variant of
first-principle molecular dynamics simulations, ADMP(Atom-centered Density Matrix Propagation). The computations of the ionic trajectories were performed for
CsCl-AlCl3 at 700 K.
RESULTS: As comprehensively reviewed in Ref. [1], up
to 1 : 1 mixture of CsCl/AlCl3 is expected to exclusively
contain AlCl4- cluster as an anion. On the other hand,
Al2Cl7− clusters were contained 9.6% of the total anions
in the whole snapshots, while AlCl4- clusters were 73.4%.
These numbers of anion rates show that AlCl4- clusters
are not always rigid, and Cl- ions are exchanged amongclusters.
Using Einstein relation for the mean square displacements versus time presented in FIG.1, self-diffusion constants were computed to be DCs = 1.216 x 10-4 cm2 s-1,
DAl = 1.530 x 10-4 cm2 s-1 and DCl = 2.671 x 10-4 cm2 s-1,
respectively. As far as we know, there is no direct reference experimental data for this system, while interdiffusion constant for NaCl-AlCl3 mixture were reported to be
4.5 x 10-6 cm2 s-1 at 413 K [2]. The square displacements
for each individual atom are presented in FIG. 2. Al atoms, center of each anion clusters, exhibit both diffusing
and static dynamics. A part of Cl atoms corresponds to Al
atoms, both for two diffusing Al’s and remaining
non-diffusing two. Nevertheless, the rest of Cl’s cannot
be categorized to either of them. This result also supportsthat Cl- ions are exchanged among clusters.
DISCUSSIONS: For CsCl-AlCl3 mixture system, anion structure of isolate AlCl4- tetrahedra shift to corner-sharing two-tetrahedron structure, Al2Cl7− , dramati-

FIG. 1 Mean square displacements versus time for
ADMP dynamics of constituent atoms at 700 K.

FIG. 2 Square displacements versus time for ADMP
dynamics of Cs, Al and Cl atoms at 700 K.
REFERENCE:[1] M. P. Tosi, D. L. Price, M.-L. Saboungi, Annu. Rev.
Phys. Chem. 44 173 (1993).
[2] B. Gilbert, D. L. Brotherton and G. Mamantov J.
Electrochem. Soc. 121 773 (1974).

採択課題番号26P11-11
ｆ－元素の有効利用に関わる基礎及び応用研究
プロジェクト（同志社大・理工）後藤琢也（京大院・エネ科）蜂谷 寛（京大・原子炉）上原章寛、藤井俊行、
山名 元62

PR11-11

Precipitation Behavior of Trivalent Dysprosium Ion by Reaction with Oxide Ion
in CaCl2–LiCl Molten Salt

H. Sekimoto, A. Uehara1, T. Fujii1, H. Yamana2

nm and 2 weak absorption peaks at 918 and at 1121. Figure 2 shows the absorption spectra of Dy3+ in
Li2O-DyCl3-CaCl2-LiCl molten salt. The spectra were
shifted upward and the difference between the top of theabsorption peak and the absorbance on the tangential line
between the feet of the peak at around 1296 nm became
smaller with introducing O2-. These indicates that theformation of DyOCl or Dy2O3(s) proceeded and theamount of Dy3+ in molten salt decreased.

Faculty of Engineering, Iwate University
Department of Materials Science and Engineering
2
Graduate School of Science, Kyoto University4Research
Reactor Institute, Kyoto University
1

0.8

-1

CDy3+ = 0.064 mol kg-1

0.6
Absorbance, A / cm

INTRODUCTION: Development of recycling technique for neodymium magnet is essentially important toachieve sustainable society. Consequently, we propose
and are investigating a new recycling process of neodymium magnet using B2O3 flux [1]. In the process, theneodymium magnet is melted together with sufficientamount of B2O3 in graphite crucible to form molten ironbased alloy, B2O3 slag and Nd2O3-B2O3 slag, which isrecovered and dissolved in molten salt. And then,Fe-Nd-B alloy is produced by electrolysis. For the process, thermodynamic properties such as solubility of rareearth oxide in molten salt is important information. In
this study, precipitation behavior of dysprosium withadding oxide ion in CaCl2-LiCl eutectic molten salt wasinvestigated by spectrophotometry.

-1

CDy3+ = 0.116 mol kg

0.4-1

CDy3+ = 0.157 mol kg

0.2

0.0
800

1000

1200

1400

1600

Wavelength,  / nm

Fig. 1. Flowchart of the recycling process for neodymium magnet proposed in this study.
2.0
1.6
2nd add-1

Absorbance, A / cm

EXPERIMENTS: Solidified samples of CaCl2-LiCl
eutectic molten salt and 5 mol%Li2O-(CaCl2-LiCl)eu.
molten salt were prepared through the following procedure. Li2O, CaCl2 and LiCl was weighted, mixed,
co-melted at 700 °C in cylindrical quartz tube andquenched in Ar atmosphere. 3.01 g of CaCl2-LiCl eutectic molten salt was inserted in a quartz optical cell andmelted at 700 °C. The intensity of the transmitted lightthrough CaCl2-LiCl eutectic molten salt using a tungsten
lamp and a spectrophotometer. Then, adding small
amount of DyCl3 in the CaCl2-LiCl molten salt andmeasuring the intensity of the transmitted light throughDyCl3-(CaCl2-LiCl)eu. molten salt was carried out repeatedly to obtain absorption spectra of Dy3+ at 700 °C.
After that, adding small amount of adding
Li2O-CaCl2-LiCl molten salt and measuring the intensityof the transmitted light through Li2O-DyCl3-CaCl2-LiClmolten salt was also carried out repeatedly to obtain absorption spectra of Dy3+ at 700 °C. Using the data on theintensity of the transmitted light, absorbance was evaluated.

1.2
3rd add

0.8

before0.4

1st add

0.0
800

900

1000 1100 1200 1300 1400 1500 1600
Wavelength,  / nm

Fig. 2. Cyclic voltammogram of CaCl2 molten salt
and CaCl2-Nd2O3-B2O3.

RESULTS: Figure 1 shows the absorption spectra of
Dy3+ in DyCl3-(CaCl2-LiCl)eu. molten salt at 700 C.
There are three absorption peak depending on the concentration of Dy3+ in the range of wavelength,  from
800 nm and 1600 nm; a strong absorption peak at 1296

REFERENCES
H. Sekimoto, A. Uehara, T. Fujii, H. Yamana, KURRI
Progress report, (2012) 102

採択課題番号 26P11-12

吸光分光測定を用いた高温融体中の金属イオンのプロジェクト
溶存形態に関する研究 (f-元素の有効利用に関わる基礎及び応用研究)（岩手大・工）関本 英弘（京大・原子炉）上原 章寛、藤井 俊行、山名 元
63PR11-12

Elucidation of the Uptake Route of Radionuclides in Deciduous andConiferous Trees Using Radio Cesium and Radio Potassium in Annual Tree Rings

T. Ohta, T. Kubota1, Y. Shibahara1, S. Fukutani1 , T. Fujii1
T. Igarashi, Y. Mahara2

the surface soil and did not penetrate deeper into the soil.
The results clearly show that radio-Cs in soil has not
moved from the tree roots to the annual tree rings because the active root system rarely was found in the surrounding surface soil. The high 137Cs concentration in thesapwood zone of konara coincided with the direction of
the arriving radioactive plume in the sampling sites.
Conversely, the concentrations of 137Cs and 134Cs in theannual tree rings of sugi showed non-directionality. As
the radioactive Cs moved from the leaves to the tree
trunk, the directionality of radio-Cs in the annual treerings was eventually disappeared. The results of the present study indicate that 134Cs and 137Cs, detected in thetree rings, from the Fukushima NPP were directly absorbed from the atmosphere by the bark and leaves rather
than the roots. Furthermore, the results suggest that theconcentrations of radio-Cs in the trees in Fukushima
would not further increase in the future.
On the basis of the distribution of radio-Cs in the annual tree rings of the both trees of konara and sugi, we
propose the following guidelines for using contaminatedwood from Fukushima when high concentrations 137Cs
have been detected in the trunk: (1) use the parts of wood
where the 137Cs concentrations are low, and (2) use thehighest parts of the trees as sources of bio-ethanol and/or
biomass, which correspond to the energy sources for the
next generation.

Faculty of Engineering, Hokkaido University
1
Research Reactor Institute, Kyoto University
2
Professor Emeritus, Kyoto University
INTRODUCTION:
Although previous studies have measured the distribution of radionuclides in tree rings, the uptake route of137
Cs originating from the fallouts of nuclear weapon
tests and the Chernobyl accident has undoubtedly argued
the roots1)-4). A number of researchers have also reported
that 137Cs and Pu are absorbed by trees through their barkand leaves; although ambiguously, conclusive evidence
has been presented5).
Understanding the uptake route of radiocesium (radio-Cs) in the annual tree rings is important for a forest
decontaminating in Fukushima. Thus, we investigated thefate of radio-Cs in the Fukushima forestry environment
to understand its uptake route using following method:
the behavior of radiocesium in the soil and the measurements of radiocesium in the annual tree rings of the deciduous tree konara and the coniferous tree sugi by
gamma-ray spectrometry.
EXPERIMENTS
Our experiment is composed three objectives: 1) depth
profile of 137Cs, 134Cs, and 40K in the observed sites, 2)
speciation of radio-Cs in soil, 3) measurement of 137Cs
and 40K in tree rings

REFERENCES:[1] Fesenko et al., Radiat. Environ. Biophys., 40, 105(2001).
[2]Goor and Thirty, Sci. Total Environ., 325, 163 (2004).
[3] Momoshima et al., J. Environ. Radioact., 22, 93(1994).
[4]Kagawa et al., J. Environ. Qual., 31, 2001 (2002).
[5]Kudo et al., J. Environ. Radioactivity, 21, 55 (1993).

RESULTS:The behavior of 137Cs in the soil samples collected in
Fukushima showed the following: (1) radio-Cs in the soil
was primarily absorbed by soil minerals within the top
1-cm-depth from the surface; and (2) 137Cs in soil waswater insoluble and >95% of 137Cs was bound to organicand residual matters. These observations suggest that the137
Cs released from the Fukushima NPP was trapped in

採択課題番号 26P11-13

福島の森林資源有効活用のための樹木年輪放射性核種の プロジェクト
取り込み経路の解明（北大・工）太田朋子、五十嵐敏文（京大・原子炉）窪田 卓見、芝原雄司、福谷 哲、藤井俊行（京都大学）馬原保典
64

Photon Activation Analysis of Alkali Earth Elements and Arsenic

PR11-13with Bremsstrahlung at the KURRI-LINAC
T. Kubota, T. Fujii, S. Fukutani, Y. Shibahara and T.
Ohta1

empirical.

Kyoto University Research Reactor Institute1
Graduate School of Engineering, Hokkaido University

INTRODUCTION: Photonuclear reaction induced byhigh energy photons can produce nuclides that are hardly
produced in a nuclear reactor, for example, neutron deficient nuclides and carrier free isotopes through (γ, n) and(γ, p) reaction, respectively. High energy photon is generated in the bombardment of electrons of 30 MeV to platinum sheets at the KURRI-LINAC. We attempted to
conduct activation analysis for silicate salt in the previous
report [1]. However, Al-29 expected in (γ, p) reaction was
not observed. The results showed the investigation ofeffective reaction cross-sections was required for various
kinds of target samples. In this report alkali earth elements are used as target sample in order to obtain carrier
free alkali metal elements, and in addition the concentration of arsenic in seaweed is evaluated as a preliminary
test instead of neutron activation [2].

Fig. 1. Apparent cross-section for photonuclear reactions; (γ, n), (γ, p) and (γ, np) reaction

EXPERIMENTS: The target samples were once heated to dehydration and disintegrate organic compounds;
alkali earth salts were dried at 100ºC; and seaweed(Hizikia fusiformis) was incinerated at 450ºC. Eachsample was encapsulated in a quartz tube [3]. The tube inan aluminum vessel was irradiated with photon generated
by electron energy of 30 MeV at average current of 200µA for 4 to 48 hours. Radioactivity, A, induced byphotonuclear reaction was measured by γ -spectrometry
and provided the apparent cross-section, θ, which is determined by the following equation:(

A = M 0θ ( µ A ) 1 − e−λt)Fig. 2. Gamma spectrometry of seaweed (Hizikia
fusiformis) irradiated for four hours at the KURRI-LINAC.

where M0, (µA), λ and t were mole number of target nuclide, average electron beam current (micro-ampere),
decay constant, and irradiation time, respectively.

REFERENCES:[1] T. Kubota et al., KURRI PROGRESS REPORT 2013(2014) CO12-5.
[2] R. Ogawa et al., Bulletin of the Faculty of Education,
Ehime University 53 (2006) 131-136.
[3] T. Kubota et al., Recent Advances in Actinide Science,
RSC Publishing (2006) 68-70

RESULTS: Fig 1 shows the apparent cross-sections as
a function of mass number. The cross-section of (γ, n)reaction was larger than that of (γ, p) reaction by one order of magnitude. While the former was the largest at
heavy element, seems to be constant between mass number of 40 to 100. The latter was almost constant independent of mass number. For a light element (γ, np) reaction was also observed; however, its cross-section was
small. The measurement of activated seaweed shows thepeaks of As-74 in Fig. 2. The cross-sections of somephotonuclear reactions were obtained for isotope production and activate analysis, even though these values are

採択課題番号 P11-14
海水中の放射性核種および重金属の濃度測定（京大・原子炉）窪田卓見、藤井俊行、福谷 哲、芝原雄司（北大・工）太田朋子
65

プロジェクトPR11-14

Study of Applicability of Isotopic Ratio Measurement for Analysis ofRadionuclide in Environmental Samplesespectively. Because of the loading amount of Sr and Cs,
the mass spectra of radioactive Cs and Sr were obtainedwith a secondary electron multiplier detector (SEM).
RESULTS: In the measurement of radioactive Cs,
135
Cs, 136Cs and 137Cs were detected (Fig.1 (a): 134Cs was
not detected, because of the amount generated by theirradiation at KUR. In this measurement, it was observedthat the isotopic ratios of 135Cs/137Cs and 136Cs/137Cs were0.9103±0.0008 and 0.00022±0.00001, respectively. Thesemean that the several ten femto-gram of Cs would be
detectable with the four orders of the significant figures.
In the measurement of radioactive Sr, 89Sr, 90Sr and91
Sr were detected at the measurement 2.6 days later. The
mass spectra of 91Sr and 89Sr were disappeared at themeasurement of 31 days later and 574 days later, becauseof the half-life of 91Sr (T1/2 = 9.5 h) and 89Sr (T1/2 = 50.5d). The obtained isotopic ratios were agreed with resultsof the estimation by using ORIGEN-II code [5]. Thismeans that the several ten femto-gram of Sr would also
be detectable.
It was confirmed that the recovery/analysis method of
Cs and Sr have the applicability for the analysis of radioactive Cs and Sr released on the accident of Fukushima
Dai-ichi Nuclear Power Plant. The loading amount ofseveral pico-grams of radioactive Cs and Sr would bringthe information of the isotopic ratio with the four ordersof significant figure until the ten periods of half-live.

Y. Shibahara, T. Kubota, S. Fukutani, T. Fujii,
T. Shibata1, M. Yoshikawa1
Kyoto University Research Reactor InstituteKyoto University Institute for Geothermal Sciences

Intensity (arb)

INTRODUCTION: For the analysis of radionuclide,the radiation measurement such as γ-spectrometry,
β-spectrometry, and α-spectrometry were mainly performed. Although these methods have been used for themeasurement of radioactive nuclide such as nuclear fuelmaterials and fission products released on the accident ofFukushima Dai-ichi Nuclear Power Plant, they may havedisadvantage in the case of the analysis of radionuclide
having the long half-life and/or that of isotopic composition including naturally occurring isotopes. Because themass spectrometry has advantage for the analysis of theisotopic composition of the elements with high accuracy,
this method may have the applicability for the analysis ofradionuclide released on the accident of Fukushima
Dai-ichi Nuclear Power Plant.
Although the amounts of radionuclide such as radioactive Cs and Sr released on this accident were very huge,
the contaminated environmental samples show the small
radioactivity per unit weight of the contaminated environmental samples, since the contaminated area is very
wide. For the study of the recovery/analysis method of
cesium and strontium, thus, the radioactive Cs and Sr
were generated by the irradiation of natural uranium at
KUR.
EXPERIMENTS: Radioactive Cs and Sr were generated by the irradiation of 10 mg of UO2 of natural uranium at the Kyoto University Research Reactor with theneutron flux for 5.5×1012 n/s cm2. The amounts of the
major radionuclide of Cs and Sr generated by the irradiation for 3 hours were estimated as 7.4×10-11 g (137Cs) and4.5×10-11 g (90Sr). About 2 days later, the irradiated sample was dissolved with 8M HNO3 and heated to dryness.
The residues were immersed in 8 M HNO3 and the insoluble residues were removed by centrifugation. TRU
elements in sample solution were removed by the extraction-chromatography with UTEVA-resin [1], and thesample solution was evaporated to dryness. The residues
was dissolved with 3 M HNO3 solution. After the recovery of Sr by the extraction-chromatography with Sr-resin[2], Cs was recovered by using with ammonium phosphomolybdate (AMP) [3]. The sample solutions for the
analysis of isotopic composition of Sr and Cs were obtained with the dissolving 1 M HNO3 (10μL for Sr, 20 μL
for Cs, respectively).
Isotopic compositions of Cs and Sr were measured
with a TIMS (Triton-T1, Thermo Fisher Scientific). A 1
μL aliquot of each solution was loaded onto a rhenium
single filament with a TaO activator [4]. Loading amountof 90Sr and 137Cs were 4.5×10-12 g and 3.7×10-12 g, re-Intensity (arb)

1

(a)

x10

x10

(b) 134

135

136

x100

137

2.6 days later(89Sr/90Sr=0.79, 91Sr/90Sr=0.012)
2.9 days later(89Sr/90Sr=0.79, 91Sr/90Sr=0.008)
30.8 days later(89Sr/90Sr=0.53)
104.7 days later(89Sr/90Sr=0.20)
573.9 days later(90Sr only)

84

85

86

87

88

89

90

91

Atomic mass [u]Fig.1 Mass spectra of radioactive Cs and Sr. (a) Cs, (b) Sr.

REFERENCES:[1] Y. Shibahara et al., J. Radioanal. Nucl. Chem., 303:
1421-1424 (2015).
[2] T. Kubota et al., J. Radioanal. Nucl. Chem. 303:
39-46 (2015).
[3] Y. Shibahara et al., J. Nucl. Sci. Technol. 51: 575-579(2014).
[4] J. L. Birck, Chem. Geol. 56: 73-83 (1986).

採択課題番号26P11-15 境試料中の放射性核種分析への同位体比分析法の適用の検討 プロジェクト（京大・原子炉）芝原雄司、窪田卓見、福谷哲、藤井俊行（京大・地熱研）柴田知之、芳川雅子
66PR11-15 Tracing Halogen and Noble Gas Recycling in the Northern Izu Subduction Zone by
Neutron Irradiation and Noble Gas Mass Spectrometry
H. Sumino, M. Kobayashi, K. Nagao, R. Okumura1,
S. Sekimoto1 and T. Fujii1

rear-arc magma is consistent with the slab melt contribution inferred from trace element and Pb-Sr-Nd-Hf) isotope compositions [7].
The high I/Cl ratios of the seafloor sediments canaccount for the enrichment of I in subduction fluids relative to sedimentary pore-fluids [1], whereas contributionsof halogens and noble gases from altered oceanic basalts
are limited.
A simple mass balance calculation of Ar isotopes forthe melt generation region beneath the Izu arc revealed
that higher subduction flux of pore water other than directincorporation with its host sediment/crust is necessary,and that serpentinized lithosphere in the subducting slab
is regarded as the best candidate if the hydration of thelithosphere by pore fluids is operating in a closed system.
The significantly smaller contributions of subducted
noble gases and halogens in the Izu arc magmas relative
to those in the mantle wedge peridotites may result froma difference in the P-T condition of the slab in each subduction zone, or from dilution by mantle-derived halogens and He when the subduction fluid induced partial
melting. The former implies a relatively small amount of
the pore-water-derived subduction fluids would be released from a cold slab at a sub-arc depth resulting infurther subduction of halogens, heavy noble gases andpotentially water, to great depths in the mantle, which
account for the seawater-like heavy noble gases observedin the convecting mantle [2].

Geochemical Research Center, Graduate School of Science, University of Tokyo
1
Research Reactor Institute, Kyoto University
INTRODUCTION:
Recent findings of subducted
halogens and noble gases with seawater and sedimentarypore-fluid signatures in exhumed mantle wedge peridotites [1], as well as seawater-derived heavy noble gases(Ar, Kr, and Xe) in the convecting mantle [2], provide
observations that allow us to investigate the processes
that control the return of volatile and highly incompatible
elements into the mantle. To verify whether and how suchsubduction fluids modify the composition of the mantle
beneath subduction zones, we are investigating noble gas
and halogen compositions of olivines in arc lavas from
northern Izu subduction zone and those of seafloor sediments and basalts from NW margin of the Pacific plate. A
combination of neutron irradiation and noble gas mass
spectrometry (NI-NGMS), an extension of Ar-Ar and
I-Xe dating methods, allows us to simultaneously determine trace amounts of halogens with naturally occurring
noble gases by use of ultrahigh-sensitive noble gas mass
spectrometry on neutron-irradiated samples [3,4].
EXPERIMENTS: The samples and standard samples
for NI-NGMS, Hb3gr hornblende and the Shallowatermeteorite were neutron-irradiated for six hours during a 5
MW operation of KUR by using the hydraulic conveyer
to convert halogens (Cl, Br, and I) to corresponding noble
gas isotopes. Noble gases in the unirradiated and irradiated samples were extracted selectively from fluid/melt
inclusions using in vacuo crushing. The evolved noble
gases were analyzed using mass spectrometry at The
University of Tokyo [5,6].

REFERENCES:[1] H. Sumino et al., Earth Planet. Sci. Lett., 294 (2010)
163-172.
[2] G. Holland and C.J. Ballentine, Nature, 441 (2006)
186-191.
[3] G. Turner, J. Geophys. Res., 70 (1965) 5433-5445.
[4] J.K. Böhlke and J.J. Irwin, Geochim. Cosmochim.
Acta, 56 (1992) 187-201.
[5] N. Ebisawa et al., J. Mass Spectrom. Soc. Jpn., 52(2004) 219-229.
[6] H. Sumino et al., J. Mass Spectrom. Soc. Jpn., 49(2001), 61-68.
[7] J.-I. Kimura et al., Geochem. Geophys. Geosys., 11(2010) Q10011.

RESULTS: MORB-like 3He/4He and halogen ratios of
the olivines indicate insignificant contributions to the Izu
arc magmas of radiogenic 4He and sedimentary-pore-fluid-like halogens, both of which are observedin the subduction fluids released from a slab at a depth of
100 km [1]. On the other hand, a clear difference in40
Ar/36Ar ratios between the Izu volcanic front and reararc, and a comparison with those of the seafloor sediments and altered oceanic crusts suggest that Ar of sedimentary pore-water origin in the subducting slab or hydrated layer of the mantle wedge is liberated continuously with depth and that it affects the noble gas compositionof the magma generation region significantly. A small
addition of the sediment-derived noble gases to the

採択課題番号 26P11-16

希ガス化法を用いた極微量ハロゲン測定による地球深部の水の起源の解明（東大院・理・地殻化学実験施設）角野浩史、長尾敬介、小林真大（京大・原子炉）藤井俊行、関本 俊、奥村 良
67

プロジェクトPR11-16

Volcanic and Tectonic History of Philippine Sea Plate (South of Japan)
Revealed by 40Ar/39Ar Dating Technique

O. Ishizuka, T. Fujii1, R. Okumura1, S. Sekimoto1

IBM arc). However, due to the paucity of geologicaland geophysical data from these basins, their origin
and history are yet unclear.
YK10-14 and YK13-08 cruises by R/V Yokosuka
investigated Palau Basin) and southern part of West
Philippine Basin obtained crucial geological and geophysical data [2] for reconstruction of the Philippine
Sea Plate. 12 dredge hauls and 4 Shinkai submersible
dives were made during these cruises. 40Ar/39Ar datingof dolerite sample from the Palau Basin crust exposedat the Mindanao Fracture Zone at c. 130oE gave aplateau age of 40.4 Ma. This result implies that the
spreading of the Palau Basin was still going on at 40.4
Ma. This age is within an age range of active spreading of the West Philippine Basin.
This year we conducted 40Ar/39Ar dating of basaltic
samples from 2 locations in the eastern part of the basin
along the Mindanao Fracture zone. Fig. 1 shows age
spectra for the 2 analyses. Sample 6K1358R11, which
was collected by Shinkai 6500 at 4564 m deep gave aplateau age comprising of 63.8% of released gas.
YK10-14 D3R14, which was collected further east along
the Mindanao Fracture Zone by dredging also gave awell-defined plateau comprising of 96.3% of released gas.
The plateau ages shown here are still temporary age because flux monitor measurement has not been completed
yet. However, these data strong imply that the age offormation of the Palau Basin closely matches with that ofWest Philippine Basin, and this result is crucial for tectonic reconstruction of this area. Final ages will also allow us to determine the direction and rate of seafloor
spreading when the Palau Basin formed.

Geological Survey of Japan, AIST
1
Research Reactor Institute, Kyoto University
INTRODUCTION:
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 isparticularly useful for dating submarine volcanics.
	  Since this is the first time to use KUR for our laboratory, we investigated neutron flux gradient and production of interfering isotopes for 40Ar/39Ar method by irradiating standard minerals and synthetic glasses as preparation for dating of unknown samples.
EXPERIMENTS: 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 uncertainty of thesample positions at irradiation. The irradiation capsulewas wrapped with 0.5 mm-thick Cd-foil before irradiation. The capsule was irradiated 2 hours at 5MW in Hyd
facility of KUR. Analyses were conducted using
40
Ar/39Ar geochronology facility at the Geological Surveyof Japan/AIST following the analytical procedure described in [1].
For the experiments described here, around 15 mg ofsample was analyzed in each analysis. Due to alterationof poorly-crystallized part groundmass, basaltic samples
were treated at 100oC on hot plate with stirrer in 6N HCl
for 60 minutes and then 6N HNO3 for 60 minutes to remove possible alteration products (clays and carbonates)
prior to irradiation. This procedure effectively separated
and concentrated fresh plagioclase in groundmass and of
microphenocryst. After this acid treatment, these separates were examined under binocular microscope before
packed for irradiation.
RESULTS: Two basaltic samples recovered fromthe northern margin of the Palau Basin, southernmost
part of the Philippine Sea plate, were studied. The West
Philippine Basin and Palau Basin are supposed to havebeen the oldest oceanic basins in the Philippine Sea Plate.
Accordingly, their origin and growth history can be a
critical constraint on the tectonic reconstruction of thePhilippine Sea Plate. These basins could have existed
prior to the Izu-Bonin (Ogasawara)-Mariana arc (IBMarc), or formed as a consequence of subduction initiation along the IBM arc (e.g., backarc basins of the

採択課題番号 26P11-17	
 Fig. 1 Age spectra for the basalts from the Palau Basin.
REFERENCE:[1] O. Ishizuka et al., Chem. Geol., 266 (2009), 274-296.
[2] Sasaki, T., Yamazaki, T., Ishizuka, O., (2014) Earth
Planet. Space, 66:83, doi:10.1186/1880-5981-66-83.

40

Ar/39Ar 年代測定による日本周辺海域の火山活動史及びプロジェクト
地殻構造発達史の解明	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 

（産総研）石塚	  治（京大・原子炉）藤井	  俊行、奥村	
 良、関本	
  俊	
 
	
 

68

PR11-17

Ar–Ar Age Determination of Minamitorishima

N. Hirano, H. Sumino1, T. Fujii2, R. Okumura2, S.
Sekimoto2

stead of 40K, were simultaneously analyzed using a
mass-spectrometer with an extraction technique of multi-step heating of approximately every 50 to 100 °C between 500 to 1500 °C.

Center for Northeast Asian Studies, Tohoku University
1
Geochemical Research Center, Tokyo University
2
Research Reactor Institute, Kyoto University

RESULTS: The irradiations of sample in KUR weredone in May, 2014. We are going to analyze the irradiatedsamples after cooling. We note that the Minamitorishima
is just only “island” in WPSP in spite of many of larger
volcanic edifices of seamount and guyot thanMinamitorishima. We have a hypothesis of different process and age to make the island in WPSP, awaiting future
analytical results

INTRODUCTION: Most of seamounts on the western
Pacific Plate formed before 70 Ma in the so-called West
Pacific Seamount Province (WPSP) which is characterized by relatively short seamount chains maybe indicating a significant short-lived hotspot system [1]. The geochronological studies of each Cretaceous seamount, on
the other hand, show the long-lived main shield stage ofvolcanism, because a seamount remained above a hotspot
for a long time (approximately 10 m.y. [2]). This may be
attributed to either of the following two possibilities: 1)
An abundant heat supply as in the superplume episode in
the Early Cretaceous [3][4][5]. 2) Slow absolute motionof the Early Cretaceous Pacific Plate (3–6 cm/yr.) [6][7].
The research cruise using R/V Yokosuka equippedwith the submersible SHINKAI 6500, was conductedaround the Minamitorishima Island on May 2010 in orderto know the detail history during the formation of theisland, where volcanic rock samples have never beenobtained before (Fig. 1). The shipboard multibeam
acoustic surveys showing the detail bathymetry discovered the volcanic cones on seamount slope and the clusters of small conical volcanoes on surrounding abyssal
plain (Oikawa and Morishita, 2009). Most of cones areseveral hundred meters in height and 1–10 km in diameter. We observed the stratigraphy of Minamitorishimausing the submersible SHINKAI 6500. Highly vesicularlavas were sampled at the volcanic cone on the seamountslope. The olivine-bearing dense lavas, on the other hand,were obtained at the steep slope beneath the lava platformin bathymetry, implying main-shield stage lavas in contrast to volcanic cones probably erupted at the rejuvenated stage during the Minamitorishima’s formation.

Fig. 1. Bathymetric map of Western Pacific.
REFERENCES:[1] A. A. P. Koppers et al., Geochem. Geophys. Geosyst.,
4 (2003) DOI | 10.1029/2003GC000533[2] N. Hirano et al., Marine Geol., 189 (2002) 371-379.
[3] K. G. Cox, Nature, 352 (1991) 564-565.
[4] R. L. Larson, Geology, 19 (1991) 547-550.
[5] R. L. Larson and C. Kincaid, Geology, 24 (1996)
551-554.
[6] R. A. Duncan and D. A. Clague, in The ocean basins
and margins, 89-121 (New York, Plenum, 1985)[7] J. W. Henderson et al., Tectonics, 3 (1984) 121-132.
[8] I. McDougall and T. M. Harrison, in Geochronology
and Thermochronology by the 40Ar/39Ar Method,(Oxford, New York, 1988).
[9] N. Iwata, Ph.D. Thesis, Tokyo Univ. (1998).
[10] K. Saito, Sci. Rep. Res. Inst. Tohoku Univ. (RITU),
Japan A40 (1994) 185-189.

EXPERIMENTS: Radiometric Ar-Ar dating is commonly used to determine the ages of submarine lavas,
because the traditional K-Ar dating is impossible to remove the alteration part in such rocks [8]. The
rock-samples prepared for dating were crushed to100-500 μm grains, and leached by the 1N HNO3 at
70-60 °C for one hour. The leached samples were irradiated by neutrons in a reactor to produce 39Ar from 39K
during a few hours. During the irradiation, samples were
packed with EB-1 biotite flux monitors [9], K2SO4 and
CaF2 as correcting factors in an aluminum capsule. They
are shielded by Cd foil in order to reduce neutron-induced 40Ar from 40K [10]. Then, radiogenic 40Ar,
daughter nuclide of radioactive 40K and parent, 39Ar in-

採択課題番号 26P11-18 新種の火山のメカニズムを解明するための 40Ar/39Ar 年代測定 プロジェクト（京大・原子炉）藤井俊行、関本俊、奥村良（東大院・理・地殻化学実験施設）角野浩史、（東北大・東北アジア研究センター）平野直人
69

PR12

Project Research on Nuclear Spectroscopy and Condensed Matter
Physics Using Short-Lived Nuclei

Y. Ohkubo

annealed in vacuum at various temperatures. Theyobserved no clear signal of such complexes in the
TDPAC spectra. However, the TDPAC spectra indicatethat Ce and He form complexes having a variety ofgeometrical structures. Comparison with TDPAC results
reported by another research group on 111Cd arising from111
In in He-doped stainless steel shows that the parent
atoms (La and Ba) of 140Ce trap He atoms more
efficiently than In atoms do, indicating stronger bondingof He to the former atoms, while different from thepresent case, 111Cd (In)‒He complexes form a uniquegeometrical structure. A part of the results are describedin the following second page.
S. Komatsuda et al. (PRS-3) investigated thermal
behavior and interacting nature of 100-ppm Al and~100-ppt In impurities doped in a semiconductor ZnO
by means of the TDPAC technique with the 111In(→
111Cd) probe. They observed the following contrasting
interactions between Al and In impurities depending on
different atmospheric conditions: (1) in air, Al and In
impurities irreversibly associate with each other in theprocess of thermal diffusion of these two species, but (2)in vacuum, these bound states formed in air dissociate byheat treatment at temperature higher than 873 K, and thedissociation reaction is enhanced with increasing
temperature. Considering that the dissociation is triggeredby the oxygen vacancy formation near the locallyassociated In‒Al structure and using the TDPAC dataobtained, they estimated the activation energy of theoxygen‒vacancy formation to be 0.72(6) eV. A part of
the results are described in the following third page.
Superionic conductivity observed for AgI emerges onlyat the high-temperature (≥ 420 K)  phase because of
temperature-dependent crystal structures, which is abarrier to the practical applications of this compound.
Recently, this problem was attacked by a novel technique:powder AgI coated with poly-N-vinyl-2-pyrrolidone(PVP) can drastically enhance the ionic transport property
at room temperature. W. Sato et al. (PRS-4) studied
dynamic behavior of the extranuclear field relative to the111
Cd(← 111Ag) probe nucleus incorporated in AgI, using
the TDPAC method. For PVP-coated AgI nanoparticles,
they observed nuclear spin relaxation of the probe atroom temperature, which indicates that Ag+ ions in the
PVP-coated sample make hopping motion from site tosite at this low temperature. From the TDPAC dataobtained, they estimated the activation energy for the
dynamic motion to be 46(10) meV. A part of the results
are described in the following fourth page.

Research Reactor Institute, Kyoto University
Objective and Participating Research Subjects
The 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 first year of the project.
Unfortunately, no experiments in all six research subjectsof the project (26P12) were executed owing to thesuspension of the reactor operation. Here, we report someresults which were obtained in previous periods and havealready been published in journals.
The research subjects (PRS) reported here are as
follows:
PRS-1  Decay of 150Ce to 150Pr
PRS-2 Interaction between He and Elements with A =140 in Fe
PRS-3 Atmosphere Dependence of Stability of Local
Fields in Al-Doped ZnO
PRS-4 Extranuclear Dynamic Motion of 111Cd(← 111Ag)
Doped in AgI Nanoparticles
Main Results and Contents of This Report
At KUR-ISOL (the on-line isotope separator installedat the Kyoto University Research Reactor), Y. Kojima etal. (PRS-1) studied the  decay of 150Ce having ahalf-life of 6.05(7) s produced by the thermal-neutroninduced fission of 235U. From -ray singles and ‒coincidence measurements, they newly found 9 excitedstates and 37-rays and constructed a decay scheme
containing 18 excited states and 55 -rays which include
the newly found excited states and -rays. They
concluded that the dominant -feeding at the 110-keV
excited state of 150Pr arising from the  decay of 150Ce to
be an allowed unhindered spin-flip transition. They
furthermore proposed the Nilsson configurations of theground state and the 110-keV excited state of 150Pr. A
part of the results are described in the next page.
In order to examine whether Ce (or rather, La and Ba)
and He form complexes having a definite geometricalstructure in Fe as suggested in first-principles density
functional theory calculations, Y. Ohkubo et al. (PRS-2)
projected 100-keV 140Cs+ at KUR-ISOL and then 4-keV
He+ using an ion beam gun into an Fe foil and tooktime-differential perturbed-angular-correlation (TDPAC)
spectra at room-temperature of 140Ce arising through140
Ba-140La from 140Cs in He-doped Fe, unannealed and

採択課題番号 26P12
短寿命 RI を用いた核分光と核物性研究（京大・原子炉）大久保嘉高
70

プロジェクト decay of 150Ce to 150Pr

Y. Kojima, K. Kosuga1, Y. Shima2, A. Taniguchi3,
H. Hayashi4 and M. Shibata

0
0

2000

4000

789

688

x5

558

1000

380

Counts2000

100

INTRODUCTION: Decay data provide valuable information about unstable nuclides. In particular, the branching ratio I is one the most important properties
from the nuclear structure viewpoint. For even-even 150Ce,
Fogelberg et al. briefly reported an intense -transition to
the 110-keV level in 150Pr [1]. If this -feeding is an allowed unhindered transition, it will lead to the assignment of the Nilsson orbital for 150Pr. However, it is uncertain whether this transition is firmly an allowed unhindered transition because of the following reasons.
First, ref. [1] did not provide detailed experimental dataon 150Ce. Second, the other published data for 150Ce arevery scarce and partly inconsistent with each other [2,3].
In the present work, decay studies on 150Ce have been
performed using the on-line isotope separator at KUR(KUR-ISOL) [4] to investigate low-energy level structures in150Pr. Note that this work was recently published[5]. This report is an outline of the paper.
EXPERIMENTS: The 150Ce nuclides were producedby the thermal neutron induced fission of 235U. The
mass-separated source was periodically moved to a detector port with time intervals of 12.2 s.
Time-dependent -ray singles and  coincidence measurements were performed with two Ge detectors in ameasurement period of 46 h. The energy and efficiency
calibrations were made using standard -ray sources.
RESULTS: The half-life and coincidence relationships
with the Pr KX-ray were analyzed to assign the parent
nuclide of each -ray observed in this work. From theseanalyses, 57 -rays including 39 new -transitions were
found to be due to the decay of 150Ce.
Energy spectra gated on the-rays from 150Ce were analyzed to establish -ray cascade relations. For example,
Fig. 1 is a spectrum gated on the 110-keV -ray. This
spectrum shows that the 110-keV -ray is coincident with
13 -rays. From these cascade relations and also fromenergy sum rules, the excited levels in 150Pr and the -ray
placements were unambiguously proposed. The decay
scheme includes 18 excited levels. Nine levels of themwere newly proposed. The 717-keV level seen in ref. [3]was not observed in this work.
The -ray intensities relative to that of the 110-keV tran-

106
169
180
200
231
279.2

Radioisotope Research Center, Nagoya University
School of Engineering, Nagoya University
2
Graduate School of Engineering, Nagoya University
3
Research Reactor Institute, Kyoto University
4
Institute of Biomedical Science, The University of Tokushima Graduate School
1

KX

sition were deduced from peak counts observed in the
singles spectrum or in coincident spectrum. Multipolarities of three -rays were also estimated from the intensity
ratio between KX and -ray peaks observed in the coincident spectrum: M1/E2 for the 103- and 154-keV -rays,
and E1 for the 110-keV -ray.
Finally, the I and log-ft values were calculated from thetransition intensity ( and conversion electron) imbalance
for each excited level. A small log-ft value of 4.9 wasobserved for the 110-keV level. It leads to spin-parity J= 1+ for this level.
DISCUSSION: The very intense -feeding to the
110-keV level is an allowed transition, and should be
explained by selection rules for -decays of deformed
nuclei [6]. Near the Nilsson orbitals observed in theneighboring nuclides, only the spin-flip transition between 3/2[532] and 5/2[532] satisfies the selection
rules. Thus, this -transition is interpreted as one of thecoupled neutron in 3/2[532] orbital in 150Ce changing toa proton in the vacant 5/2[532] orbital in 150Pr. This configuration yields J = 1+, and agrees with our spin-parity
assignment. The configuration of 5/2+[413]-3/2[521]
was also proposed for the ground state of 150Pr from thesystematics of the neighboring nuclides and from coupling rules.
CONCLUSIONS: A detailed decay scheme of 150Ce,
which includes 37 new -rays and 9 new excited levels,
was proposed from -ray measurements. On the basis of
the systematics and observation of the allowed spin-flip
transition, the Nilsson configurations were newly proposed for the ground and 110-keV level in 150Pr.

62, 63

PR12-1

6000

Channel number (0.125 keV/ch)

Fig. 1. A -ray spectrum gated on the 110-keV
-transition. Coincident -rays are indicated with
their energies in units of keV.
REFERENCES:[1] B. Fogelberg et al., Nucl. Phys. A 453 (1986) 15-25.
[2] K. Yamauchi et al., KURRI-KR-3 (1996), pp.51-53(in Japanese).
[3] K. S. Basu et al., Nucl. Data Sheets 114 (2013) 435.
[4] A. Taniguchi et al., Nucl . Instr. and Meth. A 351(1994) 378-382.
[5] Y. Kojima et al., J. Phys. Soc. Jpn. 84 (2015)
054201/1-8.
[6] G. Alaga, Phys. Rev. 100 (1955) 432-433.

採択課題番号 26P12-3

核分裂生成物に対する線直線偏光度測定を中心としたプロジェクト
核分光実験（名大・RI）小島康明、柴田理尋（名大院・工）嶋 洋佑、常少亮太 （名大・工）小菅数人（徳島大・医）林 裕晃 （京大・原子炉）谷口秋洋
71

PR12-2

Interaction between He and Elements with A = 140 in Fe
He-doped(1)140CeFe (4 × 1013/cm2 He corresponding to
only 0.0003 dpa), it is unlikely for He ions to directly
displace them. We think that He atoms diffused andbonded to the parent atoms of "good" 140Ce (interstitial
He atoms diffuse much more easily than vacancies: thecorresponding calculated activation energies are 0.06 and0.68 eV, respectively). As the dose of He increases, thenumber of the parent atoms of "good" 140Ce decreases. If
140
Ce‒He complexes take one or a few definite
geometrical structures, these would be reflected in the
TDPAC spectra and it may be possible to determine
whether He atoms are at substitutional or interstitial sites.
The observation that the oscillation amplitude is only
reduced but not damped with time under the He
implantation indicates that 140Ce‒He complexes take avariety of geometrical structures, accordingly these 140Ce
bonded by He feeling various electric field gradients due
to He. It is natural to think that many He atoms surroundthe parent atom and that there is a distribution of thenumber of He atoms attached to it.

Y. Ohkubo, A. Taniguchi, Q. Xu, M. Tanigaki and K.
Sato
Research Reactor Institute, Kyoto University
INTRODUCTION: As far as we know, the state of
impurities He and Ce in Fe has not been studied
experimentally until our recent work [1]. This knowledge
is important in materials science related to nuclear fusion
reactor materials. With a nuclear spectroscopic technique,the time-differential perturbed angular correlation (TDPAC)
technique, we obtained the result that the parent atoms(La and Ba) of 140Ce very efficiently trap He and they
form complexes in Fe, which do not have a definite
geometrical structure. The present report describes thelatter result. See [1] for the full description.
EXPERIMENTS: 100-keV 140Cs+ (~1.4 × 1012/0.2 cm2)
were projected into an Fe foil at KUR-ISOL. 140Cs decays
through 140Ba and then 140La to 140Ce. We name thissample 140CeFe. Three additional samples were preparedusing the 140CeFe. The first, second and third wereprepared by projecting 4-keV He+ of ~4 × 1013, ~5 × 1014
and ~2 × 1016/cm2 in this sequence into the 140CeFe. We
name them He-doped(1)140CeFe, He-doped(2)140CeFe
and He-doped(3)140CeFe, respectively. The profile of the
He concentration in Fe overlaps that for 140Cs.
Room-temperature TDPAC spectra of 140Ce were taken
for these four samples.

-0.10

no He
[1.93(1)Grad/s, -0.042(3)]

-0.05
0.00
-0.10

A22 G22 (t)-0.05

RESULTS: Fig. 1 (from top to bottom) shows the
TDPAC spectra obtained at room temperature for 140CeFe,
He-doped(1)140CeFe, He-doped(2)140CeFe and He-doped(3)140CeFe, all four with no annealing. The top spectrum
is the one appearing in [2]. As explained there, theoscillation pattern seen in the spectrum is due to a uniquestatic magnetic hyperfine interaction at 140Ce occupying
the Fe substitutional site with no lattice defects nearby(the Larmor frequency equals 1.927(7) Grad/s). Hereafter,
we call these 140Ce "good" 140Ce. From the value of theamplitude of the oscillation, "good" 140Ce are only about
30% of the 140Ce implanted in Fe. In Fig. 1 are also
shown the characteristic values for each oscillation
component seen in the TDPAC spectra. As the dose of He
increases to ~5 × 1014/cm2, the oscillation amplitude gets
reduced more and more (note that the amplitude is not
damped with time), and at the dose of ~2 × 1016/cm2(He-doped(3)140CeFe) no clear oscillation is observed.
The dose of 2 × 1016/cm2 corresponds to 0.15 dpa(displacement per atom) at the maximum. This large
number may imply that He ions directly displace theparent atoms of "good" 140Ce from the substitutional sites.
However, based on the fact that the oscillation amplitude
is reduced by as much as ~50% even for the

1st He irrad.
[1.90(1), -0.020(3)]

0.00
-0.10

2nd He irrad.
[1.91(1), -0.013(3)]

-0.05
0.00

-0.10
3rd He irrad.

-0.05
0.00
0

5

10

15

20

25

t (ns)

Fig. 1. Room-temperature TDPAC spectra for 140CeFe before
He irradiation, He-doped(1)140CeFe, He-doped(2)140CeFe, andHe-doped(3)140CeFe, all with no annealing. The two values inthe square brackets in each panel are the Larmor frequency(Grad/s) and the amplitude of the oscillation component.

REFERENCES:[1] Y. Ohkubo, A. Taniguchi, Q. Xu, M. Tanigaki and K.
Sato, Phil. Mag. Lett. 94, 470-477 (2014).
[2] Y. Ohkubo, A. Taniguchi, Q. Xu, M. Tanigaki, N.
Shimizu and T. Otsuka, Phys. Rev. C 87, 044324(2013).

採択課題番号 26P12-4 鉄中での不純物原子と 140Ce 不純物原子核との相互作用 プロジェクト（京大・原子炉）大久保嘉高、谷口秋洋、谷垣 実、徐 虬（京大院理）常山正幸、谷口良徳

72

PR12-3

Atmosphere Dependence of Stability of Local Fields in Al-Doped ZnO

S. Komatsuda, W. Sato1 and Y. Ohkubo2

G22 t the time-differential perturbation factor as a function of the time interval, t, between the relevant cascade
γ-ray emissions, and N(θ,t) the number of the coincidence
events observed at angle, θ. The spectrum in Fig.1(a)shows that 100 ppm Al and 100 ppt 111In are locally-associated in ZnO matrix, suggesting that there is astrong attractive force between Al and In in ZnO [1,2].
For the spectrum in Fig. 1(b), two different components
were observed: one is that appearing in the spectrum in
Fig. 1(a) and the other is that observed for undoped
ZnO[3]. This observation implies that the probe graduallyresides solely at the substitutional Zn site after annealing
under argon gas in the same way as the case for the sample heat-treated in vacuum. These observations suggestthat the drastic change of local structure formed by Al
and In ions is closely related to the presence of O2 gas. In
oxide compounds, in general, oxygen vacancies are likely
to be formed during annealing process at a lower partialpressure of atmospheric oxygen. Therefore, it is suggested that the local association of Al and 111In becomes unstable in anaerobic atmosphere due to the formation ofoxygen vacancies in the sample. For further informationon the stability of the local structure, dependence of partial pressure of oxygen for the dissociation process needs
to be investigated.

Department of General Education, National Institute ofTechnology, Ichinoseki College
1
Institute of Science and Engineering, Kanazawa University
2
Research Reactor Institute, Kyoto University
INTRODUCTION:
Impurity-induced
properties
emerging in ZnO has been attracting increasing attention
toward its application to functional materials in a wide
field of industry. For a practical use of ZnO as a conduction-controlling device, it is of great importance to study
the physical and chemical states of doped impurities
and/or oxygen vacancies. From this point of view, wehave investigated the factors determining the local structures and their stability of Al-doped ZnO samples synthesized on different conditions by means of thetime-differential perturbed angular correlation (TDPAC)
method. In a series of our TDPAC studies, drastic changeof the local structure was observed for Al-doped ZnO
sample heat-treated in vacuum [1,2]. In order to provide
further insight into the above atmosphere dependence, inthe present work, we performed an additional TDPAC
measurement for 100 ppm Al-doped ZnO annealed underargon gas flow.
EXPERIMENTS: For the synthesis of 100 ppm
Al-doped ZnO, stoichiometric amounts of Al(NO3)3・
9H2O and ZnO powder were mixed in ethanol. The suspension was heated to evaporate the ethanol until dryness.
The powder was pressed into two disks and sintered in air
at 1273 K for 3 h. For TDPAC measurements, commercially available 111In solution was added in droplets onto
the sintered disks at the concentration of 100 ppt. The
disks again underwent heat treatment in air at 1373 K for
2 h. After that, a TDPAC measurement was performed
for one of these samples prepared in air. The other sample was ground into powder and annealed under argon
gas flow at 1373 K for 24 h. A TDPAC measurement was
carried out for the 111In(→111Cd) probe on the 171-245
keV cascade γ rays with the intermediate state of I = 5/2
having a half-life of 85.0 ns.
RESULTS: Fig. 1 shows the TDPAC spectra of 111In(→
111Cd) probe in 100 ppm Al-doped ZnO annealed (a) in
air and (b) in argon gas. The directional anisotropy on theordinate, A22 G22 t , was deduced by the following relation for delayed coincidence events of the cascade:Fig. 1. TDPAC spectra of 111In( → 111Cd) in 100 ppm
Al-doped ZnO annealed (a) in air and (b) in argon gas. The
TDPAC measurements were performed at room temperature.

REFERENCES:[1] S. Komatsuda et al., J. Appl. Phys., 116 (2014)
183502/1-5.
[2] S. Komatsuda et al., J. Radioanal. Nucl. Chem., 303(2015) 1249-1252.
[3] W. Sato et al., Phys. Rev. B, 78 (2008) 045319/1-5.

2 [ N (π , t )－N (π / 2, t )]A22G22 (t ) =.
N (π , t ) + 2 N (π / 2, t )Here, A22 denotes the angular correlation coefficient,

採択課題番号 26P12-5	  	  	  金属酸化物中不純物サイトの局所構造観察	
 プロジェクト	 （金沢大・理工研究域）佐藤	  渉（金沢大院・自然）小松田沙也加（京大・原子炉）大久保嘉高	
 73

PR12-4

Extranuclear Dynamic Motion of 111Cd(← 111Ag) Doped in AgI Nanoparticles

W. Sato, R. Mizuuchi1, N. Irioka2, S. Komatsuda3, S.
Kawata4, A. Taoka and Y. Ohkubo5

were performed for the synthesized sample at various
temperatures. The directional anisotropy, A22G22(t), wasdeduced with the following relation:

Institute of Science and Engineering, Kanazawa
University
1
Graduate School of Natural Science and Technology,
Kanazawa University
2
School of Chemistry, Kanazawa University
3
Department of General Education, National Institute ofTechnology, Ichinoseki College
4
Department of Chemistry, Faculty of Science, Fukuoka
University
5
Research Reactor Institute, Kyoto University

A22G22( t) =Here, A22 denotes the angular correlation coefficient,
G22(t) the time-differential perturbation factor as afunction of the time interval, t, between the relevant
cascade γ-ray emissions, and N(θ, t) the number of thedelayed coincidence events observed at an angle, θ.
RESULTS: It was found that TDPAC spectra of the111
Cd( ← 111Ag) probe introduced in PVP-coated AgI
measured at different temperatures show exponential
relaxation of the directional anisotropy, which signifies
that the probe is dynamically perturbed by the
extranuclear field. This phenomenon is understandable
for the spectra of the sample as in the α phase (> 420 K).
What is to be noted here is that the spectral relaxation
was also observed even at room temperature. It was
found from this observation that Ag+ ions surrounding
the probe nuclei exhibit site-to-site hopping motion in the
PVP-coated AgI nanoparticle even at this low
temperature. Fig. 1 shows the temperature dependenceof the relaxation constants. From a least-squares fit to
the data with an Arrhenius-type equation, the activationenergy, Ea, of the hopping motion was successfully
estimated to be Ea = 46 (10) meV. This value shows
fair agreement with that obtained for the superionic
conductivity: Ea = 60 meV [1]. The present result issignificant in that superionic conduction can be probedwith local dynamics observed through nuclear spin
relaxation.

INTRODUCTION: Silver iodide, AgI, is a promising
metal halide showing superionic conductivity as in its αphase, and its application to functional materials such as
solid electrolytes is thus highly expected.
The
conducting phenomenon, however, only emerges atelevated temperature (> 420 K) because the crystal
structure depends on temperature; this has indeed been abarrier to the practical applications of this compound.
Recently, an epoch-making technique has broken
through this situation: powder AgI coated with
poly-N-vinyl-2-pyrrolidone (PVP) can drasticallyenhance the ionic transport property at room temperature,
recording the conductivity of 1.5 × 10 2 Ω-1 cm 1[1].
According to the report, this achievement is due tosuccessful control of the particle size as small as€ nanoscale. In addition to the property in the bulk, it isof great importance to obtain complementary informationon the site-to-site hopping motion of Ag+ ions on an
atomic scale for a detailed understanding of ionic
conductivity of this binary solid. For that purpose, inthe present work, we have applied the time-differential
perturbed angular correlation (TDPAC) technique withthe 111Cd( ← 111Ag) probe nuclei to observe dynamic
behavior of Ag+ ions. We here report successful
evaluation of the activation energy of the dynamic
motion of Ag+ ions [2,3].
EXPERIMENTS: Pd foil was irradiated with thermal
neutrons in Kyoto University Reactor to produce the
TDPAC probe. After radioequilibrium was achieved
between 111Pd and 111Ag, the Pd foil was dissolved in
HNO3 aq. solution, and carrier-free 111Ag was isolated byan anion-exchange chromatography.
The separated
111
Ag was incorporated together in PVP-coated AgI
sample when the powder sample was synthesized by
precipitation of their raw materials. We confirmed bytransmission electron microscopy that microscopic
particles with sizes of 10-100 nm were expectedly
synthesized for 111Ag-free PVP-coated AgI.
TDPAC measurements of the 111Cd(←111Ag) probe
−

10

6 -1

 (10 s )−2[N ( π , t) − N (π /2,t)] 	
  	
  (1)
.
N( π ,t) +2N (π /2,t)

Ea = 46 (10) meV

1

2

2.2

2.4

2.6

2.8

3

3

3.2

3.4

3.6

-1

1/T (10 K )Fig. 1. Temperature dependence of the relaxation constant.
The line is the result of a least-squares fit with an
Arrhenius-type equation.

REFERENCE:[1] R. Makiura et al. Nature Mater. 8 (2009) 476-480.
[2] W. Sato et al. Chem. Phys. Lett. 609 (2014) 104-107.
[3] W. Sato et al. Hyperfine Interact. 231 (2015) 107-113.

採択課題番号 26P12-6	  	 	  超イオン伝導体ヨウ化銀中 111Ag の核スピン緩和	
 	
 	
 	
 	
 	
 プロジェクト	 （金沢大・理工研究域）佐藤	  渉（金沢大院・自然）藤澤	  照功（京大・原子炉）大久保	
  嘉高	
 

74

PR13

Project Research on the Advanced Utilization of Multi-Element Mössbauer
spectroscopy for the Study of Condensed Matter

M. Seto

MAIN RESULTS AND CONTENTS OF THISREPORT: The following reports were contributed byresearch groups in this project research.

Research Reactor Institute, Kyoto University

T. Okano et al. (P13-2) have measured 57Fe Mössbauer
spectra of Cr-doped CeFePO, for which they
demonstrated a novel ferromagnetic QCP. From theobtained spectra, they showed that transition metal Cr
substitution for Fe in CeFePO gradually generates a FM
ordering of Ce sublattice and suppresses theferromagnetic ordering by further doping, whereas Fe
sublattice does not show magnetic ordering.
197
T. Yokoyama et al. (P13-3) performed Au Mössbauer

OBJECTIVES AND PERFORMED RESEARCHSUBJECTS: Mössbauer spectroscopy is a powerful andwell established method in a wide variety of researchareas, such as physical-, chemical-, biological-, andearth-sciences. As the Mössbauer resonance line isextremely narrow, hyperfine interactions are wellresolved and give us the information on the surrounding
electronic states and magnetism. The element specificinformation, which is one of the most superior features ofthe Mössbauer spectroscopy, is important and required
for modern precise materials science and complex
systems such as biological substances. Moreover,
Mössbauer spectroscopy is useful and valuable because it
usually does not demand the doping of radioactive
sources for the measured samples; the decay of theunstable nucleus sometimes induces the unwanted changeof local electronic states.
The main objectives of this project research are theinvestigation of the fundamental properties of newmaterials and the development of the advanced
experimental methods by using multi-element Mössbauer
spectroscopy under high-magnetic fields.
However, owing to the unexpected shutdown of theresearch reactor and the tracer laboratory for the long term,some of the planned researches have not been performed.
The research subjects performed are as follows:

P13-2
P13-3

P13-5
P13-6

P13-7
P13-9

spectroscopic study of manganese dioxides, and theinformation obtained from the analysis of the measured

spectra indicated a formation of Au(III) surface complex
on manganese dioxide.
To investigate the origin of the multiferroics and identify
phase relation in the ferroelectric catalysis, S. Nakamura
et al. (P13-5) studied spinel type FeCr2O4 and Sn/BaTiO3
as multiferroics and ferroelectric catalysis, respectively.
From the 57Fe Mössbauer spectrum of FeCr2O4 at 4.2 K in
applied magnetic field of 2T and the 119Sn Mössbauer
spectrum of Sn/BaTiO3 specimen at room temperature,
the electronic states relevant to multiferroics werediscussed.
T. Kamiryo, et al. (P13-6) measured Mössbauer spectra oforiented thin sections of natural magnetite to observe thedependence of absorption peak intensities on the
crystallographic orientation, and the proposed model
were discussed to explain the result.
To develop zero thermal expansion (ZTE) materials, I.
Yamada et al. (P13-7) studied the chemical substitution
effect of cubic perovskite oxide LaCu3Fe4O12 on thermal
expansion property by X-ray diffraction, thermal analysis,
and Mössbauer spectroscopy, and the obtained results
indicate that the unusual thermal expansion properties of
LaCu3Fe4–xMnxO12 are associated with valence transitionsof Fe ions.
To understand the nature of the Fe-oxipnictide
superconductors, S. Kitao et al. (P13-9) studied themagnetic
properties
oftheoptimally-doped
superconductor Ba0.6K0.4Fe2As2, and under-doped
superconductor Ba0.8K0.2Fe2As2 using Mössbauer
spectroscopy. From the obtained spectra, the co-existenceof magnetism and superconductivity was not observed in
the optimally-doped Ba0.6K0.4Fe2As2. On the other hand,
Mössbauer spectra of under-doped Ba0.8K0.2Fe2As2
showed magnetic order below around 100 K, implyingthat the superconductivity and magnetic order co-exist.

Magnetism of an iron oxypnictide Cr-doped
CeFePO (T. Okano et al.).
A study of formation of Au(III) surface complex
on manganese dioxide by 197Au Mössbauer
spectroscopy (T. Yokoyama et al.).
Mössbauer Spectroscopy of Novel FerroelectricMaterials (S. Nakamura, et al.).
Mössbauer spectra of oriented thin sections andsmall grain of magnetite single crystal(T. Kamiryo, et al.).
Electronic States of Negative/Zero Thermal
Expansion Materials (I. Yamada et al.).
Mössbauer Study of Fe-Based Superconductors,
Ba1-xKxFe2As2 (S. Kitao, et al.).

採択課題番号 26P13（京大・原子炉）瀬戸

多元素メスバウアー分光法の凝縮系研究への高度応用

誠75

プロジェクトMagnetism of an Iron Oxypnictide Cr-doped CeFePO

T. Okano, M. Matoba, Y. Sakai, A. Sakurai, H. Fujioka, A.
Wakatuki, K. Takeuchi, K. Nagamine, S. Kitao1, M. Seto1,
and Y. Kamihara(b) 1.00

(a)
1.00

300 K

0.90
300 K

1.00

Transmission

30 K

Department Applied Physics and Physico-Informatics,
Keio University
1
Research Reactor Institute, Kyoto University
INTRODUCTION: A continuous phase transition,
which is stimulated by an external pressure, magnetic
field, and/or chemical doping at zero temperature, iscalled a quantum phase transition (QPT). The criticalpoint of QPT is called a quantum critical point (QCP),
where second-order phase transitions have been suppressed to zero from finite temperatures. QCPs have attracted much attention since some materials exhibit superconductivity in chemical compositions proximity to a
QCP. [1–5] An iron oxypnictide CeFePO is a related
compound of an iron-based superconductor LaFePO [6]CeFePO is also one of heavy-fermion materials with Ce.
4f-electron’s sublattice inducing Kondo screening. [7,8]In the case of Ruderman-Kittel-Kasuya-Yosida (RKKY)
exchange interaction exceeding Kondo screening, longrange magnetic order appears. While many Ce-based
Kondo lattices show antiferromagnetic (AFM) groundstates, only few systems are known with ferromagnetic(FM) order competing Kondo screening. In CeFePO,
magnetic ordering is almost quenched and/or suppressed.
[8] For Cr-doped CeFePO, we demonstrate a novel ferromagnetic QCP. [1] These ferromagnetic metals are ofinterest in view point of hyperfine interactions and important for their use in the determinations of nuclear
magnetic dipole moments by a variety of methods including those based on low-temperature nuclear orientation.
EXPERIMENTS: Polycrystalline CeFe1-xCrxPO (x =0.000–0.692) were prepared by a solid state reaction.
Samples were characterized by X-ray diffraction (XRD),
magnetization measurements, and 57Fe Mössbauer spectroscopy (MS) at various temperatures. Magnetization
measurements were performed on a superconducting
quantum interference device (SQUID).
RESULTS:
Almost all XRD diffraction peaks are assigned to calculated Bragg positions of the CeFePO phase with spacegroup P4/nmm (No. 129), although there are several
weak peaks which can be attributed to Cr2P, Ce2O3, andCeO2. These impurities provide no significant influenceon magnetic measurements of CeFe1-xCrxPO because it
has been confirmed that they do not show ferromagnetic
phase down to 2 K. Samples contained less than 1 at.% of
Cr2P and 2 at.% of Ce2O3 for x = 0.500. However, forx>0.500, a ratio of Ce2O3 phase increases rapidly andCeO2 phase emerges. Figure 1 shows 57Fe MS of x = 0.10

0.90

1.00
4.2 K

Transmission

PR13-1

0.90
1.00
20 K

0.90
1.00
10 K

0.90
0.90
1.00

0.80

4.2 K

-4

-2

0

2

-1

Velocity (mm s )

4

0.90

-4

-2

0

2

-1

4

Velocity (mm s )Fig. 1 Observed 57Fe MS of x = 0.100 (a), 0.200 (b)for CeFe1-xCrxPO at several temperatures. Each solidline is a theoretical spectrum that includes a finite
quadrupole splitting. All MS can be fitted with nomagnetic splitting indicating paramagnetic phase of
Fe sublattice.
and 0.20 for CeFe1-xCrxPO from 4.2 K to 300 K. Our results show that transition metal Cr substitution for Fe in
CeFePO gradually generates a FM ordering of Ce
sublattice and suppresses the FM ordering by further
doping, whereas Fe sublattice does not show magnetic
ordering. The ground state of Ce 4f orbital in CeFePO is
dependent on interlayer distances.[9] Arrott plot of theM-H curves determines a ferromagnetic transition temperature (Tc) for Cr-doped CeFePO. [1]
REFERENCES:[1] T. Okano, S. Kitao, M. Seto, T. Atou, M. Itoh, M.
Matoba, and Y. Kamihara, J. Appl. Phys., 117 (2015)
17E123/1-4.
[2] C. Krellner, K. S. Kini, E. M. Brüning, K. Koch, H.
Rosner, M. Nicklas, M. Baenitz, and C. Geibel, Phys.
Rev. B, 76 (2007) 104418.
[3] E. M. Brüning, C. Krellner, M. Baenitz, A. Jesche, F.
Steglich, and C. Geibel, Phys. Rev. Lett., 101 (2008)
117206/1-4.
[4] S. Doniach, Physica B+C, 91 (1977) 231-234.
[5] K. Yoshida, A. Okiji, Prog. Theor. Phys., 34 (1965)
505-522.
[6]Y. Kamihara, H. Hiramatsu, M. Hirano, R. Kawamura,
H. Yanagi, T. Kamiya, and H. Hosono, J. Am. Chem.
Soc., 128 (2006) 10012-10013.
[7] T. Nakamura, T. Yamamoto, M. Matoba, Y. Einaga,
and Y. Kamihara, J. Phys. Soc. Jpn., 81 (2012)
064714/1-4.
[8] S. Kitagawa, H. Ikeda, Y. Nakai, T. Hattori, K. Ishida,
Y. Kamihara, M. Hirano, and H. Hosono, Phys. Rev.
Lett., 107 (2011) 277002/1-5.
[9] S. Kitagawa, K. Ishida, T. Nakamura, M. Matoba, and
Y. Kamihara, J. Phys. Soc. Jpn., 82 (2013) 033704/1-4.

採択課題番号 26P13-2
ペロブスカイト関連鉄系超伝導体の磁性
プロジェクト(慶大・理工) 岡野智宏、的場正憲、酒井雄樹、櫻井信、藤岡弘考、若月厚志、竹内勝彦、長嶺良麿、神原陽一 (京大・原子炉）北尾真司、瀬戸誠

76

PR13-2

A study of formation of Au(III) surface complex on
manganese dioxide by 197Au Mössbauer spectroscopy

T. Yokoyama1, Y. Okaue1, D. Kawamoto1, H. Ando1, H.
Ohashi2, S. Kitao3 and Y. Kobayashi3

may be fixed tightly on the surface of MnO2 due to theformation of Au-O-Mn bond (surface complex).
In conclusion, information arising from the analysis of197
Au Mössbauer spectroscopy indicated Au(III) ion adsorbed chemically to form surface complexes before
spontaneous reduction of the Au(III) to Au(0).

1Faculty of Sciences, Kyushu University
Faculty of Arts and Science, Kyushu University
3
Research Reactor Institute, Kyoto University
2

INTRODUCTION: It is known that gold nanoparticles
supported on metal oxide have been used as various oxidation-reduction catalysts. Gold catalyst made by deposition-precipitation (DP) method has been often used forcatalytic study. However, it has been still poorly understood how Au(III) ions are precipitated on the surface of
metal oxide. We have studied for Au(III) ions adsorption
on the surface of metal oxide. In our study, we concluded
that adsorbed Au(III) ions were not physically adsorption
but chemical adsorption with surface complex (M－O－
Au, M:metal). We did not prove straightforwardly theformation of Au(III) surface complex on metal oxide,
which the aim of this study is to prove by means of 197Au
Mössbauer spectroscopy.

1.00
0.99
0.98

Relative Transmission

EXPERIMENTS: Au(III) ion adsorbed on manganeseoxide was prepared by batch method. Manganese dioxide (Chuo Denki Kogyo Co., Ltd.) was added into An
aqueous solution of HAuCl4 under stirring and maintaining pH 6. The suspended solution was filtered with 0.45
μm membrane filter.
The chemical state of gold in the solid samples obtained was determined by 197Au Mössbauer spectroscopy(home-made equipment). The 197Pt isotope (T1/2 = 18.3h), γ-ray source feeding the 77.3 keV Mössbauer transition of 197Au, was prepared by neutron irradiation of isotopically enriched 196Pt metal at the Kyoto University
Reactor. The absorbers were particle specimens. The
source and specimens were cooled with a helium refrigerator. The temperature of the specimens was in therange 8 – 15 K. The zero velocity point of the spectra
was the peak point of pure bulk gold. The spectra for all
the solid samples were fitted to a single Lorentzian function.

1.00

0.99

(b)

1.00

0.99

(c)

0.98

-15 -10 -5 0
5 10 15
Velocity / mm s-1

20

Fig. 1. 197Au Mössbauer spectra for Auad/MnO2(a),KAuBr4(b) and AuMe2acac(c).

Au/MnO2RESULTS: Figure 1 shows 197Au Mössbauer spectra ofstandard materials and Au(III) adsorbed on manganesedioxides. Figure 2 shows relative absorption area estimated from spectra in Fig.1 based on area of gold plate.
The area is a measure of the recoilless fraction which is afunction of the degree of fluctuation of Au nuclei (structural hardness). In Fig. 2, area of KAuBr4 is considerably smaller than that of Auad/MnO2. The result suggeststhat Au nuclei in KAuBr4 can fluctuate more easily thanthat in Auad/MnO2, deducing that the latter Au(III) ion

採択課題番号 26P13-3

(a)

0.97

KAuBr4

AuMe2acac

0.0

0.2

0.4

0.6

0.8

1.0

1.2

1.4

Normalized Area ratio (gold plate =1.0)

Fig. 2. Normalized area ratio of 197Au Mössbauer
spectra for AuMe2acac, KAuBr4 and Auad/MnO2.

メスバウアー分光による金属酸化物上に吸着した金(III)イオンの触媒的還元反応の状態分析

プロジェクト（九大院・理）横山拓史、岡上吉広、川本大祐、安東宏晃 （九大・基幹教育院）大橋弘範（京大・原子炉）北尾真司、小林康浩
77PR13-3

Mössbauer Spectroscopy of Novel Ferroelectric Materials

S. Nakamura, J. Kano1, N. Oshime1, N. Ikeda1, Y. Kobayashi2, S. Kitao2 and M. Seto2

with the estimated direction of the magnetic moments.
Note that the quadrupole splitting e2qQ/2 changes from
-3.11 (Hex = 0) to -3.23 mm/s (Hex = 2 T), which may be
indicative of the multiferroelectricity of this material.
In Fig. 2, 119Sn Mössbauer spectrum of Sn/BaTiO3
specimen at room temperature is shown. The spectrum iscomposed of a quadrupole doublet with isomer shift of-0.015 mm/s and quadrupole splitting of 0.519 mm/s.
Thus we can identify that the supported Sn is in the formof SnO2. The absorption line width is rather large (0.879mm/s), which is a result of a distribution in quadrupole
splitting due to the particle size of nanometers.

Department of Science and Engineering, Teikyo University
1
Graduate School of Natural Science and Technology,
Okayama University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: Recently, novel materials related
to ferroelectrics have attracted much interest. One example is multiferroics that has at the same time ferromagnetic (or antiferromagnetic) order and ferroelectric order.
The other example is ferroelectric catalysis that is composed of metal nanoparticles supported on ferroelectric
particles. In order to investigate the origin of the multiferroics, or identify phase relation in the ferroelectric catalysis, Mössbauer spectroscopy is a useful probe [1-6].
In this research, we deal with a spinel type FeCr2O4 and
Sn/BaTiO3 as multiferroics and ferroelectric catalysis,
respectively. FeCr2O4 reveals a ferrimagnetic order below
around 70 K (tetragonal phase), followed by a spiralmagnetic order below 35 K (orthorhombic phase). In the
spiral magnetic state, a multiferroic state is expected. On
the other hand, Sn/BaTiO3 is expected as a new catalyst
for the exhaust emission. The phase relation of the supported Sn compound was not clear, because its amount is
too little to be identified by usual X ray diffraction.

4

absorption intensity (count)

2.7 104

2.6 10S1
S2

4

2.5 10FeCr2O4
T = 4.2 K, Hex = 2 T

4

2.4 10-10-50v (mm/s)5

10absorption intensity (count)Fig.1 57Fe Mössbauer spectrum of FeCr2O4 at 4.2 K
in applied magnetic field of 2 T.

EXPERIMENTS:
For FeCr2O4, a single crystal
specimen of (100) platelet was used as an absorber. In
order to obtain a single domain state in the low temperature phases, a slight compression along [001] axis wasadded by attaching epoxy resin on its both edges. 57Fe
Mössbauer spectroscopy was conducted in conventionaltransmission geometry by using 57Co-in-Rh (50 mCi) as γ
ray source. The spectrum was measured at 4.2 K withapplication of a magnetic field of 2 T. The direction ofthe γ ray and the magnetic field were parallel to the [100]axis. While for Sn/BaTiO3, a powder specimen was used
as an absorber. 119Sn Mössbauer spectroscopy was conducted by using 119Sn-in-CaSnO3 (20 mCi) as γ raysource. The spectrum was measured at room temperature.

5.6 106

5.55 106

5.5 1065.45 106

5.4 106

Sn/BaTiO3
at RT

-4

-3

-2

-1

0
1
v (mm/s)2

3

4

Fig. 2 119Sn Mössbauer spectrum of Sn/BaTiO3
specimen at room temperature
REFERENCES:[1] S. Nakamura et al., J. Phys. Conf. Ser. 200, 012140(2010).
[2] S. Nakamura et al., J. Phys. Soc. Jpn. 83, 044701(2014).
[3] S. Nakamura et al., J. Phys. Soc. Jpn. 84, 024719(2015).
[4] S. Nakamura et al., J. Phys. Conf. Ser. 592, 012122(2015).
[5] T. Okamoto et al., Hyperfine Interactions 219,147-152 (2013).
[6] J. Kano et al., Jpn. J. Appl. Phys. 53, 05FB24 (2014).

RESULTS: In Fig. 1, 57Fe Mössbauer spectrum of
FeCr2O4 at 4.2 K in applied magnetic field of 2 T isshown. The spectrum is composed of two subspectra,
which indicates that the magnetic structure is not a simple
cone spiral type. Although both magnetic moments lie
approximately in the orthorhombic c-plain, one is directed along the a-axis (corresponding to the cubic [100]),
whereas the other inclines about 60º from the a-axis. The
observed fields (Hobs) decrease by 2 and 1 T, respectively,
due to the applied magnetic field. This is well consistent

採択課題番号 26P13-5
新規誘電体関連材料のメスバウアー分光
プロジェクト（帝京大・理工）中村真一（岡大・自然）狩野旬、押目典宏、池田直（京大・原子炉）瀬戸誠、北尾真司、小林康浩
78

PR13-4

Mössbauer Spectra of Oriented Thin Sections andSmall Grain of Magnetite Single Crystal

T. Kamiryo, K. Shinoda, Y. Kobayashi1
The following two models were discussed to explain thisresult. In the first model, supposing that magnetic domains with the easiest magnetization axis of crystallographically equivalent <100> or <110> or <111> arepresent equally in oriented thin sections, the peak 2 ration
were always 2 in all cases. This model is not consistent
with this result. In the second model, supposing shapemagnetic anisotropy, which means possibly high magnetic domains with the magnetized orientation parallel tothe thin sections and low magnetic domains normal to thethin sections, this result can be explained only by the<111> easiest magnetization axis. This is consistent
with the general easiest magnetization axis of spinel ferrite.

Department of Geosciences,
Graduate School of Science, Osaka City University
1
Research Reactor Institute, Kyoto University

INTRODUCTION: We have made Mössbauer micro-spectrometer using a multi-capillary X-ray lense(MCX) and estimated beam size of γ-ray at the focus inorder to measure Mössbauer spectra of a single crystal in
petrographic thin sections (KURRI Progress Report2013). As powdered crystals are generally used forconventional Mössbauer spectroscopy, anisotropy of
crystal against incident γ-ray can be cancelled by randomorientation of powders, and sextet peaks due to internal
magnetic field are averaged into intensity ratio of
3:2:1:1:2:3. On the other hand, intensity ratio of sextet
of single crystal depends on the crystal orientation. In
this study, to observe crystallographic orientational dependence of sextet, Mössbauer spectra of oriented thinsections of natural magnetite were measured.

Mössbauer spectra measurements of small single grainsof magnetite with MCX were not done, because theTracer Laboratory was not opened for Mössbauer
specrtroscopy.

EXPERIMENTS and RESULTS: Two natural magnetite single crystals were prepared. Using X-ray precession camera, (100), (110) and (111) oriented thin sections
were made for Mössbauer spectra measurements. Vacancy x (Fe3-xO4, 0<x<0.33) of Brazil and Russia magnetites was estimated to approximately 0 and 0.2, respectively, from Mössbauer spectra. Peak fittings as two
sets of sextet were done for 6 thin sections. Sextet of
49T and 46T magnetic fields are shown in table as Fe3+
and Fe2.5+, respectively. Relative intensity in the table isthat of the second peak (peak 2) against the third peak
(peak 3) among separated 6 peaks. For powdered magnetites, the relative intensity of peak 2 is always 2. But
they were deviated from 2 due to crystal anisotropy.

occurrence
BrazilRussiaindex Fe2.5+ Fe3+(100) 1.96

1.72(110) 2.70

2.31(111) 2.86

2.56(100) 1.98

1.83(110) 2.73

2.64(111) 2.75

2.63

Table. Relative intensity of peak 2 against peak 3 among
sextet of magnetite.

採択課題番号 26P13-6 磁鉄鉱定方位単結晶と単粒結晶のメスバウアースペクトル測定 プロジェクト（大阪市大・理）上領卓也、篠田圭司（京大・原子炉）小林康浩	
 79

PR13-5

Electronic States of Negative/Zero Thermal Expansion Materials

I. Yamada,1 S. Marukawa,2 S. Kitao3, and M. Seto3
1

Research Institutes for the Twenty-First Century
Osaka Prefecture University
2
Department of Chemistry, Osaka Prefecture University
3
Research Reactor Institute, Kyoto University
INTRODUCTION: Positive thermal expansion (PTE)
is an essential property of materials. A limited number ofmaterials shrink with heating, which is described as negative thermal expansion (NTE). NTE property contributes
to development of zero thermal expansion (ZTE) materials, in which the thermal expansion coefficient is almost
zero. ZTE materials are desired in a wide range of applications such as precise mechanics, optics, and electronics.
We investigated the chemical substitution effect of cubic
perovskite oxide LaCu3Fe4O12 on thermal expansion
property by X-ray diffraction, thermal analysis, andMössbauer spectroscopy. Eventually, we obtained almost
ZTE in Mn-doped sample, LaCu3Fe4–xMnxO12 [1].

Fig. 1. Temperature dependence of the unit cellvolume for LaCu3Fe4–xMnxO12.

EXPERIMENTS: LaCu3Fe4–xMnxO12 samples weresynthesized under high-pressure and high-temperature
conditions of 15 GPa and 1473 K, respectively. Synchrotron X-ray powder diffraction (SXRD) data were collected at temperatures between 100 and 450 K at theBL02B2 beamline of SPring-8. 57Fe Mössbauer spectroscopy measurements were conducted at temperaturesin transmission geometry using 57Co/Rh as a radiation
source.
RESULTS: Fig. 1 shows temperature dependence of
the unit cell volume for LaCu3Fe4–xMnxO12. A systematic
trend from abrupt volume expansion/shrinkage (x =0–0.5), NTE (x = 0.75), ZTE (x = 1), and PTE (x = 1.5)
was confirmed [1]. This indicates that the thermal expansion properties of this system are adjustable by chemical
doping. Fig. 2 shows Mössbauer spectra of the x = 0.75
and 1 samples collected at temperatures between 77 and
320 K. Nonmagnetic component are predominant above
room temperature whereas magnetically split sextets are
predominant at 77 K. The isomer shift values increased
by ~0.05 mm/s at magnetic transition temperatures,
which is attributed to the Fe valence reduction by intersite charge transfer (Cu2+ + Fe4+ ⇄ Cu3+ + Fe3+). These
results indicate that the unusual thermal expansion properties of LaCu3Fe4–xMnxO12 are associated with valencetransitions of Fe ions.
REFERENCES:[1] I. Yamada et al., Appl. Phys. Lett., 105 (2014)
231906.

Fig. 2. Mössbauer spectra of LaCu3Fe4–xMnxO12 (x= 0.75, 1).

採択課題番号 26P13-7	 メスバウアー分光法を用いたプロジェクト異常高原子価Feペロブスカイト酸化物の電子状態解明	
 (大阪府大・21 機構)山田幾也（大阪府大・院理）丸川翔平（京大・原子炉）北尾真司、瀬戸誠	
 80

PR13-6

Mössbauer Study of Fe-Based Superconductors, Ba1-xKxFe2As2

S. Kitao, M. Kurokuzu, Y. Kobayashi, M. Saito, and M.
Seto

RESULTS AND DISCUSSION: Typical Mössbauer
spectra for BaFe2As2 are shown in Fig. 1. The magnetictransition was clearly observed by the temperature dependence of the Mössbauer spectra. The observed internal magnetic field reached around 5.4 T at 2.5 K. The
magnetic transition was clearly observed at around 150 K.
These values well agreed with the former report[5].
On the other hand, Ba0.6K0.4Fe2As2 showed only a single
peak spectrum down to 4 K, implying no magnetic transition occurs in optimally-doped superconductor. Thus, theco-existence of magnetism and superconductivity was notobserved in the optimally-doped Ba0.6K0.4Fe2As2. This
fact was similar to the “1111” compound,
LaFeAsO1-xFx[4]. However, Mössbauer spectra in under-doped Ba0.8K0.2Fe2As2 showed magnetic order below
around 100 K, implying that the superconductivity andmagnetic order co-exist in the under-doped
Ba0.8K0.2Fe2As2. This co-existence in some of Fe-based
superconductors is still one of the main controversial
issues. Further Mössbauer study will be performed toinvestigate this issue.

Research Reactor Institute, Kyoto University
INTRODUCTION: After the discoveries of theso-called “1111” series of Fe-oxipnictide superconductors,
LaFePO[1] and LaFeAsO1-xFx[2], several series of
Fe-based superconductors have been successively discovered and extensively investigated to elucidate themechanism of their superconductivity. Among the related
Fe-based superconductors, the so-called “122” series has
been found by K-doping (i.e. hole-doping) of
BaFe2As2[3]. This series has become one of the maingroups of Fe-based superconductors, since the various
superconductors have been found not only byhole-doping but by electron-doping and even by isovalent
doping. Such variety of superconductors provides complexity in the understanding of the mechanism of superconductivity, since the character of each Fe-based superconductor shows various different properties.
To promote the understanding of the superconducting
mechanism, studies of their Fe magnetism is one of themain approaches, since it is supposed that the Fe acts as a
key element and that the magnetism must relate to thesuperconductivity. To investigate the nature of its magnetism, 57Fe-Mössbauer spectroscopy is an essential
method. Until today, a number of Mössbauer studies onthese Fe-based superconductors have been carried out
and revealed many important facts, for example, that thesuperconductivity and magnetic order do not co-exist in
LaFeAsO1-xFx[4]. However, in Ba1-xKxFe2As2, unlike
LaFeAsO1-xFx, it is known that the superconductivity andmagnetic order co-exist in some doping region of theunder-doped Ba1-xKxFe2As2[5].
In this study, a detailed temperature dependence of
Mössbauer spectra was measured to investigate the magnetic properties of the parent compound, BaFe2As2, optimally-doped superconductor, Ba0.6K0.4Fe2As2, and under-doped superconductor, Ba0.8K0.2Fe2As2.

REFERENCES:[1] Y. Kamihara, H. Hiramatsu, M. Hirano, R. Kawamura, H.
Yanagi, T. Kamiya and H. Hosono, J. Am. Chem. Soc. 128(2006)10012.
[2] Y. Kamihara, T. Watanabe, M. Hirano and H. Hosono, J. Am.
Chem. Soc. 130 (2008) 3296.
[3] M. Rotter, M. Tegel, and D. Johrendt, Phys. Rev. Lett. 101(2008) 107006.
[4] S. Kitao, Y. Kobayashi, S. Higashitaniguchi, M. Saito, Y.
Kamihara, M. Hirano, T. Mitsui, H. Hosono and M. Seto, J.
Phys. Soc. Jpn. 77 (2008) 103706.
[5] M. Rotter, M. Tegel, I. Schellenberg, F. M. Schappacher, R.
Pöttgen, J. Deisenhofer, A. Günther, F. Schrettle, A. Loidl
and D. Johrendt, New J. Phys. 11 (2009) 025014.

1.00

1.00

120K

0.98

EXPERIMENTS: BaFe2As2 was synthesized by heatingof a stoichiometric mixture of ground Ba and FeAs in a
crucible of aluminum oxide sealed in a quartz tube, as in
the reported method[3]. K-doped Ba1-xKxFe2As2 wassynthesized similarly, except that excess amount of K
was added and heated in lower temperature. The obtainedpolycrystalline powder was characterized by x-ray diffraction and magnetic susceptibility measurements. The
superconducting
transition
wasobserved
inBa0.6K0.4Fe2As2 and Ba0.8K0.2Fe2As2 at around 30 to 40 K.
57
Fe-Mössbauer spectra were measured using a pellet of
powder sample using a 57Co source in Rh matrix with anominal activity of 1.85 GBq. The velocity scales arereferenced to α-Fe.

0.98

300K

0.96
1.00

100K

0.98

1.00
0.98

150K

0.96
0.96
1.00

1.00

77K

0.98

0.98

140K

0.96

Transmission

0.96
1.00

1.00

2.5K

0.98

130K

0.98
0.96

0.96

0.94

BaFe2As2
-3

-2

-1

0

1

Velocity (mm/s)

Fig. 1.

2

3

-3

-2

-1

0

1

2

3

Velocity (mm/s)

Typical Mössbauer spectra of BaFe2As2.

採択課題番号 26P13-9 多元素メスバウアー分光法を用いた新規材料の物性研究
プロジェクト（京大・原子炉）北尾真司、小林康浩、齋藤真器名、増田亮、黒葛真行、瀬戸誠、窪田卓見
81PR 14

Translational Research on BNCT for Clinical Application

M. Suzuki

RS1. Clinical studies on BNCTTwo research groups reported case reports treatedwith BNCT using KUR. Miyatake et al. reported avery important case report from a clinical viewpoint of
new application of BNCT. In this report, radiation-induced osteosarcoma in the skull was successfully treated with BNCT. Kat et al, reported case reports of six patients with head and neck cancer.
Yanagie et al. reported the result of
18F-boronophenylalanine (BPA) – positron emission
tomography (PET) study which was taken by breast
cancer patient with right supraclavicular lymph nodemetastasis and treatment planning study.

Research Reactor Institute, Kyoto University

Background and Objective
Using Kyoto University Research Reactor (KUR),
patients with malignant tumors greater than 500 havebeen treated with boron neutron capture therapy(BNCT). Malignant brain tumors and head and neckcancers have been main malignancies treated with
BNCT. Our laboratory (Division of Particle Radiation Oncology) has investigated the possibilities for
new applications for BNCT. According to promising
results in pre-clinical study, we have already treatedsome patients with liver cancers with BNCT and carried out clinical study on phase I study on BNCT for
malignant pleural mesothelioma (MPM).
Promising clinical results of BNCT using the research reactor encouraged us to go to further stage of
BCNT using an accelerator-based (AB) BNCT system.
Co-operation of Kyoto University Research Reactor
Institute and Sumitomo Heavy Industry have developed AB BNCT system with compact cyclotron as anaccelerator. In 2012 and 2014, clinical studies on
BNCT for recurrent malignant brain tumors and headand neck tumors to get an approval as a medical device from the Pharmaceuticals and Medical Devices
Agency (PMDA), a Japanese regulatory agency. In atransition period from reactor-based (RB) BNCT into
AB-based BNCT, many research issues should be dissolved from impending and long-term viewpoints.
Main objectives of our project is to dissolve many
impending clinical issues to perform BNCT safely in
AB-BNCT system and to investigate many research
projects for many patients with cancer to be treatedwith AB-BNCT system.

RS2. Pre-clinical studies on physiological and pharmacological aspects of BNCT
Nakamura et al. studied the effects of the countercations of boron clusters on liposome formation todevelop high boron content liposomes for BNCT byovercoming osmotic pressure limitations.
Gao et al. studied the therapeutic efficiency and suppression of the adverse effects of a novel boron-containing nanoparticles which were prepared bymixing a newly synthesized boron-cluster-containing
anionic block copolymer and a redox cationic bkicj
copolymer.
Fujimoto et al. studied the efficiency and potential of
BNCT for lung metastasis using the human clear cellsarcoma lung metastasis mouse model.
Tada et al. studied the feasibility of a boron-rich boron carbide (B4C) as a boron-including drug in BNCT
for oral cancer using xenograft nude cancer-baring
mice.
Yanagie et al. performed preclinical BNCT study for
VX-2 rabbit liver tumor model using borocaptate sodium (BSH) entrapped water-in-oil-in-water (WOW).

Research Subjects
To advance RB-BNCT into AB-BNCT, a lot of researchers in various research fields such as clinicalradiation oncology, medical physics, pharmacology,
boron chemistry, and accelerator engineering areneeded to be involved in our research projects. In
this viewpoint, this research project consists of threeresearch subjects (RS) as follows,
RS1. Clinical studies on BNCT
RS2. Pre-clinical studies on physiological and pharmacological aspects of BNCT
RS3. Medical physics studies on BNCT.

RS3. Medical physics studies on BNCT

Hayashi et al. studied the NMR response of the standard
methacrylic-acid-based polymer gel (MAGAT) with andwithout boron and examined its availability to measure
the depth-dose responses in the irradiation of neutron
beams with different energy spectra from nuclear reactor.
Tanaka K et al. reported a calculational approach formeasurement of the beam components such as thermal,
epithermal, fast neutrons and gamma rays separately using twin imaging plate system.
Sakurai et al. studied the QA/QC in BNCT using ionaization chamber and Bonner sphere in BNCT irradiation
field.
Tanaka H et al. studied the prototype system of real-time boron concentration monitor.

Main Results
Unfortunately, KUR has been unavailable since May
in 2014. Many research subjects could not be performed.

採択課題番号 26P14（京大･原子炉）鈴木 実

BNCT 実用化に向けた橋渡し研究82

プロジェクトPR14-1 Boron Neutron Capture Therapy for Radiation-induced Osteosarcoma from the Skull
S. Miyatake, S. Kawabata, R. Hiramatsu, G. Futamura
T. Kuroiwa, Y. Sakurai1, H. Tanaka1, A. Maruhashi1,
M. Suzuki1, N. Kondo1, S. Masunaga1, Y. Kinashi1 andK. Ono1
Department of Neurosurgery, Osaka Medical College
Research Reactor Institute, Kyoto University

1

INTRODUCTION: From March 2014 to May 2014,
we applied boron neutron capture therapy (BNCT) for 11
lesions in KUR. The lesions were composed of 3 recurrent
glioblastomas, 2 recurrent anaplastic astrocytomas, 4high-grade meningiomas, 1 head and neck cancer and 1
recurrent osteosarcoma from the skull. We have alreadyreported the effectiveness of BNCT for malignant gliomas,
high-grade meningiomas and head and neck cancers,
however, that for osteosarcoma is extremely rare and noreport of BNCT was found for radiation-induced
osteosarcoma. Therefore we introduce here the successfultreatment of BNCT for radiation-induced osteosarcoma
from the skull.
Clinical Presentation:
A 54-year-old female was referred to our institute fortreatment by BNCT of a recurrent radiation-induced
osteosarcoma involving the left occipital bone. Ten years
earlier, she was diagnosed with cancer of the uterine bodyand underwent resection surgery. Two years after thatsurgery, she underwent chemotherapy and whole-brain
radiation therapy (WBRT, total 30 Gy with 10 fractions)
including the cerebellum for brain metastasis. Six years
after the WBRT, she was diagnosed with aradiation-induced osteosarcoma involving the left
occipital bone, and she underwent resection surgery andsuccessive chemotherapy using methotrexate. One year
after that surgery and chemotherapy, the subcutaneoustumor appeared again in the left occipital region andrapidly enlarged over a period of only 3 months (Figure 1
A). Magnetic resonance images (MRI) showed theepidural tumor invasion (Figure 2 A and A’). Eventually,
the patient could not walk because of acutely developing
cerebellar ataxia. This tumor was diagnosed as arecurrence of the radiation-induced osteosarcoma
We performed BNCT for this radiation-induced
osteosarcoma.
At one day after the BNCT, the patient’s gait
disturbance was aggravated. Computed tomography atthat time showed aggravation of peri-lesional edema(data not shown). Remarkably, the MRI taken 4 days
after the BNCT demonstrated the definitive shrinkage ofthe mass, but the left cerebellar edema was still there(Figure 2 B and B’). We then treated the edema withdehydrators and steroids. The symptoms gradually

improved.
At only 3 weeks after the BNCT, the patient was able towalk again stably without aid. The subcutaneous tumor
was reduced dramatically without radiation injury of thescalp, with time after BNCT, as shown in Figure 1 B and
C. The only adverse effect was hair loss inneutron-irradiation field, as shown in Figure 1 C. MRI
showed the further reduction of tumor and thedisappearance of the cerebellar edema (Figure 2 C andC’), 3 months after BNCT.
We experienced only a case of successful treatment of
BNCT for radiation-induced osteosacoma. Hopefullythese potential therapeutic effects will be applicable for
non-radiation-induced osteosarcomas which are generally
refractory for other treatment modalities.

Figure 1. Marked improvement of the subcutaneoustumor at 3 weeks after the application of BNCT.
A: Just prior to the BNCT; B: Seven days after the
BNCT; C: At 2 months after the BNCT,

Figure 2. MRI of the patient’s brain before and after the
BNCT.
A,A’:Just prior to BNCT
B,B’:4 days after BNCT
C,C’: 3 months after BNCT

採択課題番号26P14-4

熱外中性子を用いた悪性脳腫瘍に対する
プロジェクト非開頭中性子捕捉療法の臨床的研究（大医大・脳外）宮武伸一、黒岩敏彦、川端信司、平松 亮、二村 元、宮田とも、大村知久（京大原子炉）小野公二、増永慎一郎、鈴木 実、近藤夏子、田中浩基、櫻井良憲, 丸橋 晃
83

PR14-2

Clinical Studies on BNCT for 6 Cases of Head and Neck Cancer

I. Kato, T. Iwagami1, N. Yamamoto2, Y. Fujita3, M.
Ohmae4, M. Suzuki5, S. Masunaga5, H. Tanaka5, M.
Nakazawa, T. Sumi, A. S. Iwai, Maruhashi5, K. Ono5, Y.
Yurarate (OS) and 9-year OS were 42% and 31%, respectively.
(3)BNCT improved QOL, PS and survival periods.
(4)Survival periods after BNCT were 1-105 months. (5)Adverse events were brain necrosis, osteomyelitis andtransient mucositis and alopecia and so on.

Dept. of Oral &Max.fac. Surg. II, Grad. Sch. of Dent., Osaka Univ.
1

Case 4: A 56-year old man with SCC at the left marginof tongue (T2N0M0) had got interstitial radiation therapy(60Gy) at the Osaka University Hospital in July 2013,
with rejection against his doctor’s recommendation of thesurgery (tongue hemi-section). About 6 months after theinterstitial radiotherapy, he had developed the left lymph
node metastasis at upper neck region (level II). However,
he had again rejected to the surgery of radical neck dissection against his doctor. During his rejection of thesurgery, the lymph node had rapidly grown more than
7cm in diameter, involving carotid vein and artery. He
had referred to our department in March 2014.
FBPA-PET study resulted that T/B ratio=4.2. The left
upper neck lymph node had treated with BNCT in May,
2014. About 3 month later, the huge lymph node hadcompletely disappeared under the CT scan. Then
6-month after BNCT, he had complaint of dyspnea. He
had seen his general practitioner and his doctor advised
him to see specialist. He had found the left lung lesions
which were seemed to be distant metastasis under the CT
scan. He had got chemotherapy for treatment of lunglesions at a hospital in his home town.

Dept. of Oral &Max.fac. Surg., Han-nan Hosp.

2

Dept. of Oral &Max.fac. Surg., Saiseikai-Senri Hosp,

3

Dept. of Oral &Max.fac.Surg., Higashiosaka General Hosp.

4

Oral &Max. fac. Surg., Rinku,General Med. Center5

Research Reactor Institute, Kyoto University

INTRODUCTION: We had first reported that six patients with head and neck cancer (HNC) had been treatedwith BNCT [1]. We also report long term (more than
5-year) clinical outcomes of our 26 patients with recurrent HNC treated with BNCT [2]. We summarized here
the latest 6 patients with HNC who had treated with
BNCT at KUR in last year in Table 1.
PURPOSES: The purpose of this study was to estimate
safety and effectiveness of BNCT for patients with advanced/ recurrent HNC for which there were no othertreatment options.
RESULTS: We also report here the latest clinical outcomes of 37 patients with recurrent HNC
All cases are advanced such as 18 (49%) out of 37 patients had developed regional lymph node metastases.
Distant metastases were developed in 10 cases (27%)
during treatment. (1) Regression rates were CR:19cases(51%), PR: 14 cases (38%), PD: 3cases (8%), NE (notevaluated):1case (3%). Response rate was 89%. (2) Mean
Survival time was 26.3months. 4-year overall survival

REFERENCES:[1] I. Kato, et al., Appl. Radiat. Isot., 61 (2004)
1069-1073.
[2] R. Barth, et al., Radiat. Oncol., 7 (2012) 146-166

Table 1. Treatment Summary of 6 Cases
Case
No.

Pt‘s Initial(Age)

Clinical Diag.
(Histopathol. Diag.)1

K・M(28)Rec.of Lt-ZK (SCC)

２

K・M(63)

Rt-op.OKK、RND, Lt-LN meta

３

A・H(51)

Rt-op.ZK,RND,BNCT, lung meta

4

I・T(56)

Post RT of Lt-ZK, Lt-LN meta

５

S・K(69)Rt-OGK(SCC)after Proton T.

S・M(69)Rec.of Rt-op.UGK, RND,

6

10B-conc.
Blood(ppm)
1st 16.7
2nd 15.0
33.3
23
22
26.5
20.0

T-max of thermal neutron (D)

T/B
ratio

Total-RBE-Dose Eq (Gy-Eq)

History of RT:
(Gy)

2.9

Fluence(E+11n/cm -2)
1.5(Left-P)
1.4(Left-A)

T-Peak Gy-Eq

Skin/Mucosa

45（2.1 ㎝）

T-deepest
Gy-E
12
15
21（5.8 ㎝）

48

23
20

3.9

2.8

50

2.8

1.8

63

26（1.6 ㎝）

8.8(6 ㎝)

4.2

2.52

60(interstitial)

50

2.1

3.79

70(Proton T.)

30

2.0

3.36

60

34

18
12
13

Irradiationtime(min.)(Dec, 2014)% Reduction (Period)
Prognosis (Survival)

5.7/11

1st 66 min.
2nd 46 min.

PR・Alive(6M)

4.4/1352

PD（2M）Alive(（9M）

2.6spine80

PR(2M),DOC(8M)7.9/1270

CR(7M),Lung meta

8.3/12

44

12/14

63

PD, DOC(3M)
CR, Lung meta,DOC(6M)

採択課題番号26 P14-5 頭頸部悪性腫瘍におけるホウ素中性子捕捉療法の臨床的研究 プロジェクト（阪大 2 口外）加藤 逸郎、岩井 聡一、墨 哲郎、中澤 光博、由良 義明（阪大工）村田 勲（慶大）岡本 正人（長崎大）梅田 博昭、柳本 惣市（りんくう医療セ）大前 政利（東大阪総合）
千足 浩久（市立池田）大西 徹郎（田中クリニック）田中 善（山口大）上山 吉哉、内田 堅一郎（京大炉）田中 浩基、鈴木 実、櫻井 良憲、増永 慎一郎、丸橋 晃、小野 公二
84

PR14-3

Boron Uptake in Tumour of Local Recurrenced Breast Cancer by 18F-BPA
Positron Emission Tomograpy for Application to Boron Neutron Capture Therapy
Atomic Research Ractor 4. This simulation was performed optimizing modification to detect the minimum
thermal neutron fluence.

Yanagie H1,2,3, Furuya Y1,4, Taniike K5, Kumada H6,
NakamuraT7, Horiguchi H7, Maruyama S8, Hatae R8,
Suzuki M9, Ono K9, Ono M3,10, Nakajima J3,11, Eriguchi
M1,8, and Takahashi H2,3

RESULTS: The blood boron concentration (ppm) andtumour/normal tissue ratio are estimated to 24, 2.26, respectively. Skin RBE dose is ristricted to 10 Gy-Eq, themaximum tumour RBE dose, minimum tumour RBE
dose, and mean tumour RBE dose are 38.5, 19.9, and30.6 Gy-Eq, respectively, in 40 minutes irradiation(Figure 2). In this study, we showed the possibility toapply BNCT to local recurrenced advanced breast cancer
with the estimation of boron accumulation using
18F-BPA Positron Emission Tomograpy.

1

Department of Innovative Cancer Therapeutics: Alphaparticle & Immunotherapeutics, Meiji Pharmaceutical
University, 2Department of Nuclear Engineering &Management, Graduate School of Engineering, The University of Tokyo, 3Cooperative Unit of Medicine & Engineering, The University of Tokyo Hospital, 4Departmentof Surgery, Satukidai Hospital, 5Department of Radiology,
Nishijin Hospital, 6Department of Physics, Tsukuba University, 7Japan Atomic Research Institute, 8Department ofSurgery, Shin-Yamate Hospital, 9Research Reactor Institute, Kyoto University, 10Department of Cardiac Surgery,
The University of Tokyo Hospital, 11Department of Thoracic Surgery, The University of Tokyo Hospital
INTRODUCTION: Boron neutron capture therapy(BNCT) is a targeted radiation approach, because tumour cells can be selectively irradiated according to theaccumulation of boron compounds. The cytotoxic effectof BNCT is due to the nuclear reaction between 10B andthermal neutrons. The resulting lithium ions andα-particles have high linear energy transfer and produce
significant biological effects. Their short range in tissue(5 – 9 μm) restricts radiation damage to cells containing
boron atoms at the time of neutron irradiation. If sufficient boron compound can be targeted accurate to thetumour, BNCT can be applied to locally recurrenced gastrointestinal cancers, and breast cancers.
Recently, positron emission tomograpy(PET) is developed for primary detection and metastasis of cancers. 18F
labeled borono-phenylalanine (BPA)-PET are applyed toevaluate the accumulation of boron atoms to tumours andthe actibity of cancer cells in the fields of BNCT.

Figure 1. 18F-BPA PET image of rt cervical LN
metastasis.

CASE REPORT: We had experienced the 18F-BPA PET
for the case of breast cancer patient who had metastased
to right supraclaviclar lymph node. The patient who had
been performed modified radical mastectomy with lymph
node dissection (Patey’ s method) and adjuvant chemotherapies, had been occurred right cervical LN metastasis
after 3 years. The high accumulating images of metastased to right supraclaviclar lymph node was acquired by
18F-BPA PET. The tumour / blood ratio was 2.26 (Figure1). There was no other active images in the body.

Figure 2. Image of Patient View from frontal side
REFERENCES:[1] Y Imahori et al., Clin Cancer Res. 4(1998 )1833-41.
[2] Y Imahori et al., Clin Cancer Res. 4(1998 )1825-32.
[3] H Yanagie et al., Applied Radiation & Isotopes,
67(2009) S63-66.

EXPERIMENTS: In this case of advanced breast
cancer, we performed the feasibility estimation of 3D
construction of tumour according to the PET-CT imaging
of a patient with epithermal neutron mode at Japan

採択課題番号26P14-8 中性子捕捉療法の一般外科領域難治性癌への展開に向けた臨床的研究 プロジェクト（明薬大）柳衛宏宣、野中泰政（結核予防会新山手病院）江里口正純、小山和行、大野烈士、丸山正二、波多江 亮（宏仁会メディカルシティ東部病院）東 秀史、瀬口浩司（京大・原子炉）小野公二、増永慎一郎、
鈴木 実、櫻井良憲

85PR14-4

High Boron-Accumulated Liposomes as Efficient Boron Carriers for
Neutron Capture Therapy

H. Nakamura1, S. Tachikawa2, S. Kikuchi1, K. Ono3 and
M. Suzuki3

sionelectronmicroscopy
analysisof
spd-BSH-encapsulating
liposomes
andNa2BSH-encapsulating liposomes was also carried out
with Cryo-TEM (Fig. 2). It is notable that the liposomes
interacted with each other in the case of
Na2BSH-encapsulating liposomes, whereas the liposomes
dispersed in solution without interacting with each otherin the case of spd-BSH-encapsulating liposomes.

1

Chemical Resources Laboratory, Tokyo Institute ofTechnology
2
Faculty of Science, Gakushuin University
3
Research Reactor Institute, Kyoto University
INTRODUCTION: Boron neutron capture therapy(BNCT) has been attracting growing interest as one of theminimally invasive cancer therapies. The accelerator-based BNCT is now undergoing phase I clinical study
for the treatment of brain tumor and head and neck cancer patients using L-BPA in Japan. We previously developed Na2BSH-encapsulating 10% distearoyl boron
lipid (DSBL) liposomes that have high boron content
with excellent boron delivery efficacy to tumors.[1] In
this report, we studied the effects of the counter cationsof boron clusters on liposome formation to develop highboron content liposomes for BNCT by overcoming osmotic pressure limitations.

Fig. 2. TEM images of Na2BSH-encapsulating liposomes(left) and spd-BSH-encapsulating liposomes (right). Scale bar represents 200 nm.
Fig. 3 shows the survival curve of tumor-bearing mice
after thermal neutron irradiation. Thermal neutron irradiation enhanced mouse survival and all mice exposed tothermal neutron irradiation died within 78 days. Remarkable antitumor effect was observed in the micetreated with spd-[10BSH]-encapsulating liposomes at thedose of 30 mg [10B]/kg; 100% of the mice survived up to
100 days after the thermal neutron irradiation.[2]EXPERIMENTS: An aqueous solution of various ammonium chloride salts (1,4-diaminobutane, spermidine,and spermine) of closo-dodecaborates Na2[B12H12],Na2[B12H11OH] and Na[B12H11NH3] in addition to
Na2BSH (Fig. 1), were prepared by adding sodium closo-dodecaborates to a mixture of each amine and aqueous
1N HCl solution. Liposomes encapsulated with theseammonium closo-dodecaborates were prepared from
DSPC, cholesterol and DSPE-PEG (1:1:0.11, molar ratio)by the reverse-phase evaporation method. B/P (boron
concentration / phosphorus concentration) ratio was calculated from data obtained by the simultaneous measurement of boron and phosphorus concentrations by inductively coupled plasma atomic emission spectroscopy(ICP-AES, HORIBA, Japan).
2 Na+

SH

2-

2 Na+

H

2-

2 Na+

OH

2-

Na+

NH3

1"

Survival"rate

0.8"

Na2[B12H12]Na2[B12H11OH]

0.4"
0.2"
0"

-

0"

10" 20" 30" 40" 50" 60" 70" 80" 90" 100"Days"a9er"irradia;on"(d)

Fig. 3. Survival curve of tumor-bearing mice after thermal neutron irradiation. The irradiation was performed 36
h after injection of closo-dodecaborates (▬ , spd-BSH: 30
mg[10B]/kg; ◆ , spd-BSH: 15 mg[10B]/kg; ◇ ,spd-10B12H11NH3: 15 mg[10B]/kg) for 50 min (1.3-2.2 ×
1012 neutrons/cm2). ×, Cold control; ●, Hot control.

=B= BH
Na2BSH

0.6"

Na[B12H11NH3]

Fig. 1. Structures of closo-dodecaborates used for encapsulation in liposomes.
RESULTS:
Various ammonium salts of closo-dodecaborates were prepared and examined their encapsulation into liposomes. Interestingly, the B/P ratio
dramatically increased to 3.4 when spermidinium (spd)cation was employed. In addition, liposome yield wasmarkedly increased to 98% and final boron concentrationof the liposome solution reached 13,867 ppm. Transmis-

REFERENCES:[1] H. Koganei, et al., Bioconjugate Chem. 24 (2013)
124-132.
[2] S. Tachikawa, et al., Chem. Commun. 50, (2014)
12325-12328.

採択課題番号 26P14-16 中性子捕捉療法のための新規ホウ素薬剤の開発	
 プロジェクト	 （東工大・資源研）中村浩之、菊地俊介（学習院大・理）立川将士（京大・原子炉）小野公二、鈴
木実	
 

86

PR14-5

Boron Carbide Particle as a Boron Compound for BNCT in vivo

S Tada1, T Iwagami2, Y Ishikawa3, N Koshizaki4, H
Tanaka5, S Masunaga5, Y Sakurai5, I Kato1, K Ono5, M
Suzuki5, Y Yura1
Osaka University Graduate School of Dentistry
Hannan Municipal Hospital3
National Institute of Advanced Industrial Science andTechnology
4
Graduate School of Engineering, Hokkaido University
5
Research Reactor Institute, Kyoto University
1

2

Figure 1: Nude mice carrying SAS tumors received 50µl of 250 ppm B4C solution intratumorally. Ten
minutes later, tumors were exposed to thermal neutrons. The experimental groups were as follows: untreated control, neutron only, and B4C-mediated
BNCT. n=5

INTRODUCTION: We determined whether a boron-richboron carbide (B4C) nanoparticle could be used for
BNCT for oral squamous cell carcinoma (SCC) xenografts in nude mice.
EXPERIMENTS: B4C nanoparticles were obtained by
the laser fragmentation of boron particles in ethyl acetate
and dissolved in PBS. To generate tumors, SAS cells derived from oral SCC were inoculated subcutaneously into
the back of the leg of female Balb/c nude mice. Fifty microliters of B4C solution containing 12.5µg B4C particles
was infiltrated into tumors. 10B concentrations in thesetissues were measured by prompt gamma-ray spectrometry at the Kyoto University Research Reactor (KUR).
After injection of B4C solution, tumors were exposed tothermal neutrons. Control tumors were left untreated.
Experimental groups included untreated control, neutron
only, and B4C-mediated BNCT groups. Neutron irradiation was delivered via a neutron beam at the KUR.
RESULTS: Injecting B4C particles into the oral SCC
xenografts of nude mice increased the concentration of
10B in the tumors, but not in the kidney, liver, or spleen.
Ten minutes after injection of B4C particles the 10B
concentration was 18.57 ppm in the tumor. SAS tumor-bearing animals received an intratumoral injection of
B4C solution followed by neutron irradiation. No significant differences were observed in body weight among
these groups during the experimental period (Figure 1).
In control animals, tumors continued to grow and were5867 mm3 42 days after the start of the experiment.
When tumors were subjected to B4C-mediated BNCT,
tumor volume decreased from 7 days after neutron irradiation. A significant difference was observed between the
B4C -mediated BNCT and neutron only groups 42 days
after BNCT (P<0.01) (Figure 2).
CONCLUSION: These results indicate that B4C particles
can be used locally as a boron compound in BNCT for
oral SCC in vivo.

採択課題番号 26P14-1

Figure 2: Nude mice carrying SAS tumors weretreated as described in Figure 1. After BNCT, tumor
size was measured and tumor volume was determined. *P< 0.01 significantly different from neutrons only. n=5References[1] Ishikawa Y, Shimizu Y, Sasaki T, Koshizaki N(2007) Boron carbide spherical particles encapsulated ingraphite prepared by pulsed laser irradiation of boron inliquid medium. Applied Physics Letters 91:161110.
[2] Ishikawa Y, Sasaki T, Koshizaki N (2010) Submicron-sized boron carbide particles encapsulated in turbostratic graphite prepared by laser fragmentation in liquid medium. J Nanosci Nanotechnol 10:5467-5470.
[3] Yamamoto N, Iwagami T, Kato I, Masunaga S, Sakurai Y, et al. (2013) Sonoporation as an enhancing
method for boron neutron capture therapy for squamouscell carcinomas. Radiat Oncol 8:280.

ᝏᛶ⭘⒆࡟࠾ࡅࡿ࣍࢘⣲୰ᛶᏊᤕᤊ⒪ἲ࡟㛵ࡍࡿᇶ♏◊✲ プロジェクト（阪大・歯）多田晋也、加藤逸郎、由良義明、（阪南・歯）岩上隆紀、（京大・原子炉）田中浩基、
櫻井良憲、増永慎一郎、鈴木実、丸橋晃、小野公二
87PR14-6 Boron Neutron Capture Therapy Selectively Destroys Human Clear Cell Sarcoma (CCS)
Metastasis to Lung in CCS-bearing Animal Model
T. Fujimoto1, T. Andoh2, Y. Sakurai3, K. Ono3,
H. Ichikawa2 and M. Suzuki3

paraffin-embedded, and HE stained according to standard
protocols for histological examination.

1

Hyogo Cancer Center,
Department of Orthopaedic Surgery
2
Faculty of Pharmaceutical Sciences and Cooperative
Research Center of Life Sciences,
Kobe Gakuin University
3
Research Reactor Institute, Kyoto University

RESULTS: The irradiation doses (Gy) absorbed by the
CCS-bearing mice were 5.2 (Group A, BNCT), 0.7(Group B, Hot control) and 0.9 (Group D, γ-ray). In thethree control groups, no significant anti-tumor effect wasobserved; the tumor mass simply increased
time-dependently. By contrast, the volume of the tumor
mass in the BNCT groups decreased with time [Fig. 1].

INTRODUCTION: Sarcoma metastasis to the lung isalmost the final status for the treatment of sarcoma, andpalliative therapy is recommended for reducing severe
patient symptoms. Since neither chemotherapy nor radiation therapy is effective for most sarcomas, new therapeutic strategies are required. Clear cell sarcoma (CCS)of tendons and aponeuroses is one such with poor prognosis [1]. We have, however, demonstrated the effectiveness of boron neutron capture therapy (BNCT) for tumors
in the limbs of the human CCS-bearing nude mousemodel with the use of p-boronophenylalanine (BPA) [2,3]. Here, therefore, we first created a new model of sarcoma metastasizing to the lung in the human
CCS-bearing animal model, and then evaluated the efficacy and potential of BNCT after measuring the distribution of BPA in the lung.

CONCLUSION: BNCT selectively destroyed CCS cells
in the lung of the human CCS-bearing animal model byirradiating the whole lung, without significant complications.

EXPERIMENTS: (1) Creating the lung metastasis
model of human CCS-bearing animal model: All animal
experiments were carried out according to the regulationsof the Animal Care and Use Committee. Lung metastasis
in the human CCS-bearing animal model was created bytransplanting cells of CCS cell line (MP-CCS-SY [4])suspended in Matrigel® into the parenchyma of the left
lung of nude mice. After 8 weeks, tumor formation in thelung was confirmed by micro CT scans, and the tumor
mass was measured through CT image analysis.
(2) In BNCT trials, the animals were divided into fourgroups of 4 each, and, under anesthesia, BPA-Fr (24 mg
10B/kg) was intravenously administered to the BNCT
group (A) and to the Cold control group (C), and saline to
the Hot control group (B) on day 0. Groups A and B werethen irradiated two times with a thermal neutron beam
(1MW) to the whole lung at KURRI, once anteriorly
between 60 and 80 minutes and once posteriorly between
100 minutes and 120 minutes. The γ-ray group (D) was
irradiated with cobalt-60 γ-ray at a dose of 0.3 Gy/min.
On day 21, the tumor mass was resected from eachmouse under anesthesia, routinely formalin-fixed,

採択課題番号 26P14-19[Fig.1] BNCT for the lung metastasis model of
CCS-bearing animal model. a: Before neutron irradiation.
A well-defined solid tumor mass about 2 mm in diameter
was detected in the left lung. b, c and d: three weeks after
the neutron irradiation. b: Group A. BNCT. Tumor mass
shrank and was hardly discernible. c: Group B. Hot control. Neutron irradiation without administration of BPA.
Tumor mass was almost 3 mm in diameter. d: Group C.
Cold control. Without neutron irradiation. Tumor mass
was almost 4 mm in diameter. e: Group D. Three weeks
after theγ-ray irradiation. Tumor mass was almost 4 mm
in diameter. Bar = 2.5 mm.
REFERENCES:[1]F.M. Enzinger, Cancer, 18(1965) 1163-1174.
[2]T. Fujimoto et al., Appl. Radiat. Isot. 73(2013) 96-100.
[3]T. Andoh et al., Appl. Radiat. Isot.
69(2011)1721-1724.
[4]H. Moritake et al., Cancer Genet. Cytogenet.,
135(2002) 48-56

悪性末梢性神経鞘腫および明細胞肉腫

プロジェクトに対するホウ素中性子捕捉療法の検討（京大・原子炉）鈴木実、櫻井良憲、小野公二（兵庫県立がんセンター・整形外科）藤本卓也（神戸学院大・薬）安藤 徹、市川 秀喜

88PR14-7

Nanoparticle-assisted boron neutron capture therapeutics:
Design of novel boron-containing nanoparticle for
ROS scavenging ability improving therapeutic efficiency with low adverse effectZhenyu Gaoa,b, Yukichi Horiguchia, Kei Nakaib,
Akira Matsumurab,, Minoru Suzukic, Koji Onoc,
Yukio Nagasakia, b, d*

BNCT effect was evaluated by using tumor bearing
BALB/c mice given BNP at dose of 15 and 5 mg
10
B/kg body weight 72 h before irradiation. Micegiven boronophenylalanine (BPA)-fructose complex at dose of 40 mg 10B/kg body weight and PBS
2.5 h before irradiation were used as positive andnegative control. Tumor volume growing was monitored. White blood cell levels were confirmed 3 dafter irradiation.

aGraduate School of Pure and Applied Sciences,
University of Tsukuba,bGraduate School of Comprehensive Human Sciences, University of TsukubacResearch Reactor Institute, Kyoto University,d
WPI-MANA, NIMSRESULTS: The size of the BNP was evaluated bydynamic light scattering (DLS), showing average
size of 35 nm and neural surface. In the in vivo
BNCT effect evaluation study, the tumor volume in
PBS treated group grew up to 1.3 cm3 13 d after
irradiation. In contrast, the growth of tumors was
effectively suppressed in the BNP treated groups(average size was about 0.4 cm3, while the doses of10
B were 15 and 5 mg/kg). The suppression of tumor
growth was also observed in the mice treated by
BPA with dose of 10B at 40 mg/kg, (average size
was 0.7 cm3). By much lower dose, 5 mg 10B/kg (5ppm boron in tumor tissue), BNP showed better
therapeutic effect compared with BPA. Furthermore,
we observed high white blood cell (WBC) level in
BPA treated group, indicating the inflammation was
occurred. However the WBC level in BNP treatedgroup (15 mg/kg) showed almost similar as the
non-tumor-bearing healthy mice, probably becauseof the ROS scavenging ability of BNP. These results
strongly indicates that this novel boron-containing
nanoparticle is a suitable potential candidate forhigh performance of BNCT improving the therapeutic efficiency with low adverse effect

INTRODUCTION: Boron neutron capture therapy(BNCT) has attracted much attention during recent
decades. The success of BNCT is dependent on theboron delivery system to achieve high specific tumor accumulation, keeping low adverse effect.
However, the low molecular weight boron compounds currently used in clinical trial of BNCT are
excluded rapidly from the blood circulation, whichcauses non-specific dispersing in whole body. It is
confirmed that high-dispersion stable nanoparticle
tends to accumulate in tumor environment due tothe leaky neovascularization and immature lymphatic systems, which is called enhanced permeability and retention (EPR) effect1. Furthermore, during
the treatment process, large amount generated reactive oxygen species (ROS) will cause adverse effectsuch as inflammation. The objective of this study is
to design a novel boron nano-delivery-system thatenhance the therapeutic efficiency as well as suppress the adverse effect.
EXPERIMENTS: The novel boron-containing
nanoparticles (BNP) in this study was prepared bymixinga
newly
synthesizedboron-cluster-containing anionic block copolymer(PEG-b-PMBSH) and a redox cationic block copolymer (PEG-b-PMNT) via the ion complex inphosphate buffered saline (PBS) solution. The

REFERENCES:[1] Y. Matsumura, H. Maeda, Cancer Research 46:
6387–92 (1986)

	 採択課題番号 P14-20	
 高い腫瘍選択性を有するボロン化合物ナノ粒子の創製とプロジェクト
中性子捕捉療法への展開	
 （筑波大院・数理）高	  振宇、堀口諭吉、長崎幸夫（筑波大院・人間）中井	
  啓、松村	  明（京大・原子炉）鈴木	
  実、小野公二	 89

PR14-8 Evaluation of Component in WOW Emulsion as Intra-arterial Boron Delivery Carrier for
Neutron Capture Therapy to Hepatocellular Carcinoma
Hironobu Yanagie1,2,3, Mitsuteru Fujihara4, Ryuji Mizumachi5, Yuji Murata5, Yuriko Sakurai1,3, Kikue Mouri1,3,
Atsuko Shinohara6,7, Takehisa Matsukawa7, Yasuyuki
Morishita8, Masashi Yanagawa9, Syushi Higashi10, Ichiro
Ikushima11, Kouji Seguchi10, Sho Yui1,3,Yoshinori Sakurai12, Hiroki Tanaka12, Minoru Suzuki12, Shinichiro
Masunaga12, Kazuyuki Oyama13, Takayuki Nakagawa14,
Ryohei Nishimura14, Koji Ono12, Minoru Ono3,15, Jun
Nakajima3,16, Masazumi Eriguchi13, and Hiroyuki
Takahashi2,3patic artery (10BSH : 75 mg/kg rabbit) on VX-2 rabbit
hepatic tumour models. One and three days after arterial
injections, the boron concentrations of the tumor nodules
and normal liver tissues were determinated by ICP- Mass
Spectroscopy of Jyuntendo University.
RESULTS: VX-2-bearing rabbits (n = 3) were given
intra-arterial injection with 2 ml of 10BSH WOW emulsion consist with surfactant HCO40, or PGCR. We
prepared 10BSH entrapped WOW.
The mean 10B10
concentration prepared in BSH-WOW was 10000 ppm
in this experiment. The size of WOW was controlled to
70 μm. The 10B concentration in VX-2 tumour was 170.8
ppm, 58.3 ppm by WOW with HCO40 after day1, day3
inta-arterial injection, respectively. The 10B concentration of tumour was 186.0ppm, 40.4ppm by WOW with
PGCR after day1, day3 same injection, respectively. 10B
concentration in normal liver tissue / blood were 8.0 /0.3 ppm in HCO40 group, and 15.1 / 0.1 ppm in PGCR
group at day 3, respectively in the same procedures ofWOW. We also perform Oil-O Red staining to detect thelipid components in WOW. We had showed the stainingof cytoplasms in the tumours 3 day after itra-arterial injections(Figure 1) . These means that the WOW accumulated selectively to the tumours by intra-arterial injections.

1

Department of Innovative Cancer Therapeutics:Alphaparticle & Immunotherapeutics, Meiji Pharmaceutical
University, 2Department of Nuclear Engineering &Management, Graduate School of Engineering, The
University of Tokyo, 3Cooperative Unit of Medicine &Engineering, The University of Tokyo Hospital, 4SPG
Techno Ltd. Co., 5Department of Pharmacology,
Kumamoto Institute Branch, LSI Medience Ltd Co,
6
Department of Humanities, The Graduate School of
Seisen University, 7Department of Hygines, Faculty of
Medicine, Jyuntendo University, 8Department of Human& Molecular Pathology, Graduate School of Medicine,
The University of Tokyo, 9Department of Small Animal
Surgery, Veterinary Medical Center, Obihiro University ofAgriculture & Veterinary Medicine, 10Department ofSurgery, Ko-jin Kai Medical City East Hospital,
11
Department of Radiology, Miyakonojyo Metropolitan
Hospital, 12Department of Veterinary Surgery, The
University of Tokyo Veterinary Hospital, 13Research
Reactor Institute, Kyoto University, 14Department ofSurgery, Shin-Yamanote Hospital, 15Department of
Cardiac Surgery, The University of Tokyo Hospital,
16
Department of Thoracic Surgery, The University ofTokyo Hospital.

Day 1

Day3

NormalLiver

INTRODUCTION: We has been used water-in-oil-in-water emulsion (WOW) as the carrier of anti-cancer agents by modifying of IPSO on intra-arterial
injections in clinical. Higashi et al prepared a long term
inseparable, WOW for use in arterial injection therapy totreat patients with HCC [1]. We performed preclinical
BNCT study for VX-2 rabbit tumour model using 10BSH
entrapped WOW [2, 3]. In order to improve the WOW for
application to BNCT, we prepared 10BSH entrapped
WOW in verifying the component of surfactant, andevaluated the boron delivery activity to measure the 10B
concentrations of organs in VX-2 hepatic tumour modelon time course after intra-arterial injection.

TumourFigure1: IPSO component in WOW was accumulated inthe VX-2 tumour by intra-arterial injection of 10BSH
entrapped WOW with HCO40 surfactant by Soft X ray
radiography.
REFERENCES:[1] S Higashi S et al., Cancer, 75(1995):1245–1254.
[2] S Mikado et al., Nucl. Instr. and Meth. A, 605 (2009)171-174.
[3] H Yanagie et al., Biomedicine & Pharmacotherapy,
submitted.

EXPERIMENTS: 10BSH entrapped WOW were administrated with intra-arterial injections via proper he-

採択課題番号26P14-22

中性子捕捉療法の一般外科領域難治性癌への応用に向けたプロジェクト
DDSの基礎的研究（明薬大）柳衛宏宣、伊藤智子（東大）Novriana Dewi、柳川将志、櫻井由里子、毛利きくえ（大阪市大）長崎 健、吉川亮平、櫻本昌士（京大原子炉）小野公二、鈴木 実、櫻井良憲、田中浩基

90PR14-9

Establishment of QA/QC Using Ionization Chamber andBonner Sphere in BNCT Field

H. Ueda, Y. Sakurai, T. Takata, H. Tanaka, R. Uchida, T.
Kawamura, N. Fujimoto, M. Suzuki
Research Reactor Institute, Kyoto University
INTRODUCTION: After the restart of the operation of
Kyoto University Reactor (KUR) in May 2010, 235 clinical studies of boron neutron capture therapy (BNCT)
have already been carried out as of May 2015 [1]. Also,
the BNCT clinical trial using Cyclotron-based BNCT
Epi-thermal Neutron Source (C-BENS) started in November 2012 [2]. In the while, the research and development into several types of accelerator-based irradiation
systems are underway by several research groups in theworld at present time. With this situation in mind, it isimportant that the physical and biological estimations fordose quantity and quality are performed consistently
among several irradiation fields, and that the equivalencyof BNCT is guaranteed, even across BNCT systems. The
aim of this research is the establishment of quality assurance and quality control (QA/QC) using ionizationchamber and Bonner sphere in BNCT irradiation field. In
2014, the improvement of the energy resolution in
epi-thermal neutron region was studied for the Bonner
sphere using boric acid solution moderator.

Fig. 1. Unfolding results in the case that the activation detector displacement of 3 mm occurs on the
10-cm diameter Bonner sphere and the error is notconsidered in the unfolding procedure.

METHODS: The Bonner sphere in this research consistsof a spherical neutron moderator shell and activation foils
placed in the sphere center as thermal neutron detector.
The boric acid solution of 10B 0.14wt% was used as themoderator material. Manganin (55Mn) and gold (197Au)
were used as activation foil material. The specific saturated activities per neutron flux for each energy groupwere calculated as the response function of Bonner
spheres. The calculations were performed for the spherediameter of 10, 15 and 20 cm, using the MCNP-5 radiation transport code [3]. The calculated activities were
unfolded into the estimated spectrum by UMG unfolding
package [4]. The influence of the uncertainty for themoderator concentration and the detector placement tothe spectrum estimation, were investigated. The spectrum
estimation was performed for the epi-thermal neutron
irradiation mode in Heavy Water Neutron Irradiation Facility (HWNIF) of KUR was studied.

Fig. 2. Unfolding results in the same case as Fig. 1
except the error is considered.
REFERENCES:[1] Y. Sakurai et al., Nucl. Instr. Meth. A 453 (2000)
569-596.
[2] H. Tanaka et al., Nucl. Instr. Meth. B 267 (2009)
1970-1977.
[3] X-5 Monte Carlo Team, LA-UR-03-1987 (2003).
[4] M. Reginatto, The ’Few-Channel’ Unfolding Programs in the UMG Package (Physikalisch-Technische
Bundesanstalt) (2004).

RESULTS: Figure 1 shows the results in the case that theactivation detector displacement of 3 mm occurs on the
10-cm diameter of Bonner sphere. The error was notconsidered in the unfolding procedure. Figure 2 shows
the unfolding results in the same condition as Fig. 1, except the error was considered. In Fig. 1, the neutron energy spectrum is estimated wrongly. In Fig. 2, the neutronenergy spectrum is estimated more adequately, but theerrors of the estimated spectrum become larger.

採択課題番号 26P14-26

ＢＮＣＴ用照射場における電離箱およびプロジェクトボナーボールを用いたＱＡ／ＱＣの確立（京大・原子炉）櫻井良憲、田中浩基、鈴木 実、藤本 望、上田治明、内田良平、川村徳寛
91PR14-10

Study on the Real-time dose Monitor System Using Prompt Gamma Rays
for Boron Neutron Capture Therapy

H. Tanaka, Y. Sakurai, N. fujimoto, T. Takata, S.
Masunaga, K. Ono, A. Maruhashi, and M. Suzuki

direction, the patient was set between 0 cm and 60cm.
The background of gamma rays were produced by the1
H(n,)2D reactions with the energy of 2.22MeV, the annihilation gamma rays of 0.511 MeV, and the decay
gamma rays of 41Ar. The gamma rays at the near the collimator center are almost of 2.22 MeV produced in thehuman body. For the lateral direction, the level of gamma
rays were rapidly reduced. On the other hand, at the distance from the center of 60 cm, the dose rate of beam
direction was two times higher than that of lateral direction. This was caused by the 41Ar or annihilation gamma
rays produced by the reaction between thermal neutron
and the component of irradiation bed. Therefore, for the
beam direction, the level of gamma rays was slowly decreased. If the real-time boron concentration monitor isset at the BNCT field, it is recommended to set at thebehind of collimator for the lateral direction.

Research Reactor Institute, Kyoto University
INTRODUCTION: Over 500 clinical studies of boron
neutron capture therapy (BNCT) have been performed
using Kyoto University Research Reactor (KUR). The
information of neutron flux and boron concentration during the irradiation is needed for the determination of irradiation time. The boron concentration is determined by
the prompt gamma rays from the blood sample using
thermal neutron guide tube at KUR. On the other hand,neutron flux is measured by the activation material,
which is irradiated by the treatment beam and picked up
after 10 minutes from the irradiation start. However, theinformation of boron concentration and neutron flux is
not be able to be obtained during the irradiation. In orderto determine precise dose information, it is important todetect real-time boron concentration and neutron flux.
Recently, the real-time neutron flux monitor have beendeveloped using the combination of tiny scintillator andoptical fiber. The real-time boron concentration monitor
have been studied using SPECT system for BNCT[1].
However, the actual level system have not realized, because the background of gamma rays at the BNCT irradiation field is quite high. The aims of this study are toclarify the gamma rays dose level at the BNCT irradiation field and the development of the prototype system ofreal-time boron concentration monitor. The measured
gamma rays dose during BNCT clinical studies is shownin this report.

Fig. 1. Schematic layout of BNCT irradiation fieldof KUR and the setting position of TLDs.

EXPERIMENTS: The BeO thermoluminescence dosimeters (TLDs) were used for the measurement of
gamma rays dose. BeO powder was enclosed in quarts
tube to reduce the neutron sensitivity. The TLDs were set
at the position that was assumed to set the real-time boron concentration monitor. Figure 1 shows the schematiclayout of irradiation field and the TLDs setting positions.
The TLDs were set from the center of collimator for thelateral and beam direction with the 20 cm interval. The
height of TLDs setting position was the 60 cm, corresponding to beam center height. The irradiation was performed for head and neck tumor. The irradiation time was
63 minutes. After the irradiation, TLDs were processedby the TLD reader and the gamma rays dose were derived
with the correction.

Fig. 2. The relationship between gamma rays dose
rate and the distance from the center of collimator.
REFERENCES:[1] T. Kobayashi et al., Medical Physics, 27, 2124(2000)

RESULTS: Figure 2 shows the gamma rays dose rate
distribution for lateral and beam direction. For the beam

採択課題番号 26P14-27 BNCT のための即発ガンマ線によるリアルタイム
線量評価システムに関する研究

プロジェクト（京大・原子炉）田中浩基、櫻井良憲、藤本望、高田卓志、増永慎一郎、小野公二、丸橋晃、鈴木実

92PR14-11 Quality Assurance of Irradiation Field for BNCT Using Twin Imaging Plate System
Kenichi Tanaka, Yoshinori Sakurai1, Tsuyoshi Kajimoto,
Hiroki Tanaka1, Takushi Takata1, Jun Takada2,
Minoru Suzuki1, Satoru Endo

the beam component to the total of the energy deposition.
Here, the configuration “A-B” means that the energy
deposition for the converter ‘B’ is subtracted from thatfor ‘B’. “50% B – 10% B” or “Epoxy –Graphite” is notsuitable to use since some of the components have negative value in contribution.
In using two IPs, “50% B – Epoxy or Graphite” is potential for nepi, while 20 % of the energy deposition is byunintended component, nth. On the other hand, combining“10% B – Epoxy or Graphite” and “10% B – 1% B”, i.e.
using triple IP in Epoxy converters at 0, 1, 10 wt % of 10B,
will work in estimating nth and nepi.

Graduate School of Engineering, Hiroshima University
Research Reactor Institute, Kyoto University
2
Center of Medical Education, Sapporo Medical University
1

INTRODUCTION: Measurement of the spatial distributions of neutrons and gamma rays is one of the potentialand essential options for the quality assurance and quality
control for boron neutron capture therapy (BNCT). It is
desirable to measure the beam components such as thermal, epithermal, fast neutrons (nth, nepi, nf) and gamma
rays (), separately. This study investigates using the twin
imaging plate (IP) system for this purpose. A calculational approach is reported here.

ThermalEpithermal
Fast
Gamma

1 mm thick Epoxy
Energy deposition(MeV/sec/mA)

1000000
100000CALCULATIONS: The twin IP system consists of theconverters to enhance the components, and IPs. The principle is: thermal and epithermal neutrons will be enhanced with the secondary particles of the 10B(n,)7Li
reaction in the epoxy resin doped with boron, fast neutrons with the recoiled protons from the epoxy resin,
gamma rays with Graphite, then enhanced components
will be detected with the IPs. By comparing two IPs, intensity of a beam component is to be estimated[1,2].
The configuration of the converters was surveyed using
Monte Carlo calculations with PHITS 2.52[3]. The irradiation field assumed was that by the 7Li(p,n) reaction by
2.5 MeV protons moderated with 20 cm thick D2O. The
calculation geometry consisted of an IP (Fujifilm corporation, BAS-TR) and a converter. The IP in dimension of
20 X 20 mm was assumed to be covered with 1 mm thickconverter[1] in every direction of the IP. Each beam component was separately impinged on the converter as aparallel beam perpendicular to the IP. The epoxy resin
assumed was its compound with B4C, where boron wasenriched 10B with abundance of 100 %. The 10B concentration in epoxy resin (wt%) was varied in calculations.

10000
1000
100
0.01

10

0.1

1

10

100

B concentration in Epoxy (% )Fig. 1. Energy deposition for Epoxy at varied 10B concentration.
1 mm thick Epoxy

Ratio to total

1

ThermalEpithermal
Fast
Gamma

0.1
0.01
0.001
0.01

10

0.1

1

10

100

B concentration in Epoxy (% )Fig. 2. Beam component contribution to energy deposition.
Table 1 Energy deposition ratio (%) to total for subtraction among two IPs in converters.
Contribution (%)
Configuration
nth
nepi
nf

10% B –
50
50
00Epoxy or Graphite
50% B –
2080
00Epoxy or Graphite
10% B – 1% B
28
72
0
0
50% B – 10% B
-100
200
0
0
Epoxy – Graphite-14-5-43 162“x %B” specifies the epoxy resin with B4C at x wt% of
10
B to total weight of the converter.

RESULTS: The energy deposition in IP is shown in
Fig. 1. Those for Graphite converter is 425, 546, 1570,
and 13300 MeV/sec/mA for nth, nepi, nf, and , respectively. The contribution of each beam component to totalof the energy deposition is shown in Fig. 2. Again, thosefor Graphite is 0.3, 0.4, 1.2, 98.1 % for nth, nepi, nf, and 
In usage in twin IP system, it is desirable that only one
beam component has different energy deposition among
two IPs while other components have identical values,
respectively. In this viewpoint, Epoxy converters with 1
to 50 wt% of 10B will be potential options for detecting
nth, nepi.
Consequently, potential combinations of twin IPs arelisted in table 1. The values shown are the contribution of

REFERENCES:[1] K. Tanaka et al., Appl. Rad. Isot. 88 (2014) 143-146.
[2] K. Tanaka et al., Appl. Rad. Isot. 69 (2011) 1885-1887.
[3] H. Iwase et al., Jour. Nucl. Sci. Technol. 39 (2002)
1142-1151.

採択課題番号 26P14-28
プロジェクトイメージングプレートを用いた BNCT 照射場ビーム成分ごとの 2 次元分布品質保証（広島大・工）田中憲一、遠藤暁（京大・原子炉）櫻井良憲、田中浩基、（札幌医大）高田純
93

PR14-12

Development and Evalution of 3D Polymer Gel Dosimeter for the
Measurement of dose Distribution in BNCTS. Hayashi, Y. Sakurai1, M. Suzuki1, M. Narabayashi1and N. Fujimoto1

tron beams of the different energy spectrum modes. In
the thermal neutron mode, both profiles of the gels withand without boron show monotonically decreasing withdepth after the peak near the surface. It seems that thedecrease for the gels with boron corresponds to decreasing of thermal neutron in tissue and the peak shifts tonear the surface significantly due to the reaction withboron. In the epi-thermal and fast neutron mode, broad
peaks are observed at deeper position, around from 20 to
25 mm of depth. It is suggested that the R2 profile for the
gel with boron corresponds to the distribution of thethermal neutron due to the moderation of epi-thermal
neutron. But for the gels without boron, it seems that thedecreases correspond to decreasing of gamma ray. As
same as the profiles in thermal mode, the peak shift due
to boron was also observed. The depth profiles of themixed mode (not shown) were similar to that of thermal
neutron. It is suggested that the contributions of
epi-thermal and fast neutrons are small compared to thatof thermal neutron. These results indicate both MAGAT
gel dosimeters with and without boron have the effective
sensitivity on the thermal neutron rather than on fastneutron.

Department of Clinical Radiology, Hiroshima International University
1
Research Reactor Institute, Kyoto University

INTRODUCTION:
Polymer gel dosimeters havebeen investigated for the three-dimensional (3D) dose
measurement of the complex conformal dose distributions in the clinical applications [1]. These devices utilize
radiation-induced polymerization reactions of vinyl
monomer in the gel to preserve information about theradiation dose. The 3D absorbed dose distribution is deduced from the polymer distribution measured by imaging modalities, such as MRI. The applications to neutron
irradiation have been investigated, and the potential as a
3D dosimeter has been suggested [1].
In this work, the NMR response of the standard
methacrylic-acid-based polymer gel (MAGAT) with andwithout boron was examined its availability to measure
the depth-dose responses in the irradiation of neutron
beams with different energy spectra from nuclear reactor.

(These results were presented at 8th International
Conference on 3D Radiation Dosimetry : IC3DDose2014 in Ystad, Sweden. [2])EXPERIMENTS: Boric acid, B(OH)3, containing 10Bof 20% naturally was added into the standard gel The
concentration in the gel is the same order (approximately
50 ppm) as the clinical use. The resulting solution was
subdivided by pouring into quartz tall beakers (65 mm
diameter and 135 mm length, 400 mL).
The neutron irradiations were performed using Heavy
Water Neutron Irradiation Facility (HWNIF) of Kyoto
University Research Reactor (KUR, power of 1 MW) .
The samples were irradiated from the bottom direction
through the axis with the field size of almost 50 cm diameter in air at room temperature. The three different
modes (thermal neutron rich, epi-thermal and fast neutron rich, and the mixed modes) of neutron beams madeby heavy water spectrum shifter and cadmium thermal-neutron filters were applied to each sample.
MRI measurements were performed using a 1.5 T
scanner (Siemens). A multiple spin-echo sequence wasapplied and the transverse relaxation rate (R2 = 1/T2) was
estimated.

MAGAT/B(OH) 3 (Thermal)
MAGAT/B(OH) 3 (Epi−thermal and fast)
MAGAT (Thermal)
MAGAT (Epi−thermal and fast)3∆R 2 (/s)

2

1

0

0

20

40

80
60
Depth (mm)

100

120

Figure 1 The depth from phantom surface vs. ΔR2[=R2 – R2,bg ] responses in different energy spectra.
REFERENCES:[1]
C. Baldock et al., Phys. Med. Biol. 55 (2010)
R1–63
[2]
S. Hayashi et al., J. Phys.: Conf. Ser. 573 (2015)
012074(4pp)

RESULTS: Figure 1 shows the depth-R2 profiles obtained from our polymer gel dosimeters exposed to neu-

採択課題番号 26P14-29	
 BNCT における吸収線量分布測定のためのプロジェクトポリマーゲル 3 次元線量計の開発と特性評価	 （広国大・保健医療）林慎一郎（京大・原子炉）櫻井良憲、鈴木実、楢林正流、藤本望	
 94

I-2. Collaboration Researches
1.
2.
3.
4.
5.
6.
7.
9.
10.
11.
12.

Slow Neutron Physics and Neutron Scattering
Nuclear Physics and Nuclear Data
Reactor Physics and Reactor Engineering
Material Science and Radiation Effects
Geochemistry and Environmental Science
Life Science and Medical Science
Neutron Capture Therapy
TRU and Nuclear Chemistry
Health Physics and Waste Management
Accelerator Physics
Others95

CO1-1Analysis of Heavy Metal Elements in Chinese Medicine and Herbs

E. Furuta, N. Iwasaki, R.Okumura1 and Y. Iinuma1

structure of the 2 Chinese medicines of total 7 samples,
which were produced in China and Japan.

Ochanomizu University

RESULTS and DISCUSSION:

1

Jiedu Pian, 3 samples produced in China, were contained

Research Reactor Institute, Kyoto University

All of Niuhuangfrom 2.2 to 8.6% of As and from 1.2 to 74 ppm of Hg.
The main mineral was realgar by XRD, and the chemical
INTRODUCTION:

Chinese medicines and herbs

structure of As was sulphide; As4S4. We could not findwere analyzed in a previous experiment at KUR. At thatthe products except for Chinese one. On the other hand,results, toxic elements of As and Hg were contained withamong 4 samples, 2 of Liushen Wan were produced inhigh concentrations in 2 Chinese medicine; Niuhuang

China, and contained approx. 7% of As and 7.5% of Hg.

Jiedu Pian and Liushen Wan. However, when they are

Also, among 2 Japanese Liushen Wan, one for child wassulphide, they were not absorbed into the body. So, thecontained approx. 1% of As and 30ppm of Hg, and one

chemical structures are very important. Furthermore, low

for adult was contained approx. 550 ppm of As and 1.2

concentrations of Hg were contained in many Chinese

ppm of Hg. The main minerals of these 2 Chinese

medicines and herbs. However, Chinese medicines andLiushen Wan were realgar and cinnabar by XRD; As4S4

herbs produced in Japan contained these toxic elements

and HgS. On the other hand, the main minerals of these 2

rarely. The previous experiment raised mainly 3 queries;

Japanese Liushen Wan were gold and calcite by XRD; Au

1. Do the same named medicines contain same toxic

and CaCO3. So, the same named medicines neverelements with same level concentrations? 2. Whatcontained same toxic elements with same levelchemical structures were the As and Hg? 3. Do notconcentrations. Because the chemical structures were

Chinese medicines and herbs produced in Japan containsulphide, they are not absorbed into a body, but justtoxic elements? The purpose of this study was to clear

given a shock for the body. So, toxicity of the elements

these issues.

was no problems. Additionally, some minerals in Chinese

EXPERIMENTS:

Additional samples used in thismedicines tended to contain other toxic elements like Co,

study were 30. (The total sample number was 149.) They

Cr and Sb by INAA. Furthermore, almost all herbs

were grinded into powders with an agate mortar andcontained low level concentration of Hg. It was

enclosed each in a double polyethylene bag byconsidered the sources of Hg of low concentrations were

measuring their weight. The standard samples used werenot

JA-2 and JR-2 of rock standard, and 50 ppm of As, Hg,

contamination in the air.

Sb, Co and Cr of atomic absorption reagents (Wako)

Conclusion:

were used applying to 5 filter papers (Advantec 5A). The

medicine contained high concentration of toxic elements

samples and the standards were irradiated 1MW × 30

and many herbs contained low concentration of Hg;

min at KUR. After cooling among 5 to 10 days, thehowever, it was considered their chemical structures

gamma-rays of medium and long half life radionuclides

were not dangerous. At the same time, the safety images

were measured. Also, a XRD was used to study chemicalof Chinese medicines and herbs were not correct.

mineralsbutgrounddust

It was clarified that some Chinese

採択課題番号 26001
漢方薬、薬草に含まれる重金属元素の分析（お茶の水女子大学）古田悦子 （京大・原子炉）奥村良、飯沼勇人

96

contamination or

通常採択

Status Report 2014 for B–3 Beam Port of KUR
been refined on the basis of a cubic CaF2-type structurewith a = 4.288(1) Å, using X-ray diffraction with Cu Kα
radiation (see Fig. 2(b)). As shown in Fig. 2(a), we succeeded to observe several Bragg reflections for the(Ti0.31Cr0.33V0.36)D1.7 on the B–3 beam port; which could
be indexed on the basis of λ = 1 Å. Note that the Braggreflections correspond to the D–D correlations because of
the null alloy.
Furthermore, the data acquisition group of the neutronscience division of KEK (KEK–KENS DAQ group) has
used the B–3 beam port to assess their new 6Li-glass neutron detector system, LiTA12. The LiTA12 system consists of a 6Li-glass neutron detector with a multianodephoto multiplier tube (MA–PMT), an amplifier, and ananalog-to-digital converter (ADC) board. The B–3 beam
port has a wide space around the sample position; therefore we can easily install any other system like the
LiTA12 system.

K. Mori, H. Yoshino, Y. Iinuma, T. Fukunaga, Y. Kawabata, S. Sato1, H. Hiraka1, K. Iwase2, Y. Yamaguchi3, K.
Enjuji4, K. Furuta4, and T. Kasai4
Research Reactor Institute, Kyoto University (KURRI)
1
High Energy Accelerator Research Organization (KEK)2
Department of Materials and Engineering, Ibaraki University
3
Institute for Materials Research, Tohoku University
4
Graduate School of Engineering, Kyoto University
INTRODUCTION: The B–3 beam port of Kyoto University Research Reactor (KUR) had long been used as afour-circle single-crystal neutron diffractometer (4CND).
For the last decade, however, the 4CND was so old thatits research activity on neutron science was quite low.
Therefore, the 4CND needed to be replaced and a newneutron diffractometer has been required at the B–3 beam
port. Also, the new neutron diffractometer (Compact
multipurpose neutron diffractometer) is critical for the
structural investigations of energy storage materials suchas hydrogen absorbing alloys and rechargeable lithium-ion batteries. The neutron (powder) diffraction is a
powerful tool to determine the positions of light elements(e.g., hydrogen and lithium) in solids. Here, we report thecurrent status of the B-3 beam port of KUR and the preliminary neutron diffraction experiments using a hydrogen absorbing alloy.

(a)

INSTRUMENT: The compact multipurpose neutron
diffractometer is now being installed on the B–3 beam
port. The neutron wavelength (λ), which is monochromatized by the (220) plane of a Cu single crystal, is 1 Å. To
cover the detector area (6 º ≤ 2θ ≤ 150 º), 24 3He tube
detectors (1/2 inch in diameter) have been prepared. The
distances from the monochromator to the sample andfrom the sample to the detector will be 1.9 m and 1.2 m,
respectively. Fig. 1(a) shows the goniometer for thecompact multipurpose neutron diffractometer; we performed an operation check. A detector bank including the
24 3He tube detectors will be placed on an arm of thegoniometer. In addition, the new beam shutter was installed at the B-3 beam port, as shown in Fig. 1(b).

(b)

Fig. 1. Current status of the B-3 beam port of KUR: (a)new goniometer for the CMND and (b) new beam shutter
installed at the B-3 beam port.

(b)
4000

110

1000

400

2000

Observed data
Calculated data

200

3000

220

420

Intensity / counts

500

400

220

1000

Observed data
Calculated data

222

Intensity / counts

1500

311
222

(a)
200

CO1-2

70

90

0
FCC

0

Laves

PRELIMINARY EXPERIMENTS: The preliminary
neutron diffraction experiments were performed using thehydrogen absorbing alloy, (Ti0.31Cr0.33V0.36)D1.7, where D
is the deuterium. It is worth noting that Ti0.31Cr0.33V0.36 isa null alloy for neutron scattering due to its atomic compositions (i.e., bc[Ti0.31Cr0.33V0.36] = 0; bc[Ti] = –3.370 fm,
bc[Cr] = 3.635 fm, and bc[V] = –0.443 fm), where bc isthe coherent scattering length. The crystal structure has

20

30

40

50

2θ / °

60

70

40

50

60

80

100

2θ / °

Fig. 2. Neutron and X-ray diffraction data for a hydrogenstorage alloy, (Ti0.31Cr0.33V0.36)D1.7, collected at (a) theB-3 beam port of KUR and (b) a X-ray diffractometerwith Cu Kα radiation.

	 採択課題番号 26007	
  材料研究および中性子検出器開発を目的とした	
  	
  	
  	
  	
  	
  	
  	
  	
  通常採択
共同通常	
  	
 
	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 	
 小型多目的中性子回折装置の建設	
 （京大・原子炉）森一広、吉野泰史、飯沼勇人、福永俊晴、川端祐司（高エネ研）佐藤節夫、平賀晴弘（茨城大・工）岩瀬謙二（東北大・金研）山口泰男（京大院・工）延壽寺啓吾、古田幸三、笠
井拓矢	
 
97

CO1-3Synthesis of Metal Nanoparticles under the Gamma-ray Irradiation Field(JEOL JEM-2000FX). Samples for TEM observations
were made by putting a drop of colloidal solutions on acarbon film with a Mo mesh and dried them in a vacuum.

F.Hori, T.Hori, A.Tohkai, H.Nakanishi, A.Iwase,
M.Sakamoto2
Dept. of Mater. Sci., Osaka Prefecture University
1
Research Reactor Institute, Kyoto University

RESULTS:
Figure 1 shows the UV/vis absorption spectra for
aqueous solutions before and after gamma-ray irradiation.
It appears only one absorption peak around 570 nm,
which shows pure Cu nanopartcles production, after
gamma-ray irradiation. This is quite different from theresult that of adding of DEG [1]. This result clearlyshows that only pure Cu nanoparticles were generated
and no oxidation takes place during gamma-ray
irradiation. This is because ethylene glycol act as the
scavenger of oxidation radicals from H2O by gamma-ray
irradiation radiolysis. TEM observation shows thatgenerated particles are monodispersive spherical shapeand its average diameter is about 17 nm (fig. 2).

INTRODUCTION: It is known that metallic
nanoparticles have some specific properties, which are
not appear in bulk materials such as catalytic activities,
magnetic properties and so on. Also the character of them
depends on its size, shape, structure, chemicalcomposition and so on. For instance, it is known that Au
nanoparticles exhibit the surface plasmon resonances(SPRs) in specific wavelength at about 520 nm. They
have many possibilities to applied for various industrial
fields. Generally, many kinds of metal nanoparticles
commercially are synthesized by using chemical reaction
method. On the other hands, it has been reported thatspecific feature of metallic nanoparticles can besynthesized under energetic irradiation fields, such as
ultrasonic, electron, gamma-ray, plasma and so on. Using
these irradiation reduction methods, it is possible tofabricate the unexpected structured nanoparticles. So far,
we have successfully synthesized Cu nanoparticles,
which is not easy to reduce in aqueous solution bychemical reaction, by using gamma-ray irradiation
reduction method [1]. However, many of them are not
only pure Cu but also copper oxides. In this study, we
have tried to fabricate pure Cu nanoparticles by adding of
ethylene glycol instead of diethylene glycol.

Fig. 1 UV/vis absorption spectra of aqueous solutions

including Cu-ions
irradiation.

EXPERIMENTS: Aqueous solutions with a given
concentration of copper complex ((CH3COO)2Cu·H2O)
with an additive of of sodium dodecyl sulfate (SDS) andethylene glycol (EG). The solution was argon gas purged
and sealed into polystyrene vessels. They were irradiatedat about 300 K with 1.17 and 1.33 MeV gamma-rays
from 60Co radio active source at gamma irradiation
facility in KURRI, Kyoto University. The total dose was
fixed to 23.4 kGy with dose rate of 15.6 kGy/h. UV–vis
absorption spectra were measured by using Shimadzu
UV-2550 spectrophotometer in the wavelength range in
300-800 nm and the shapes and the structures for all
colloidal products were observed by conventional TEM

beforeandafter

gamma-ray

Fig. 2 TEM image of synthesized Cu nanoparticles by

gamma-ray irradiation reduction.
References[1] T.Hori, K.Nagata, A.Iwase and F.Hori, Jpn. J. Appl. Phys.
53(5), 2014	 採択課題番号 26010	
  	
  ガンマ線照射還元を利用した貴金属ナノ微粒子の創成（阪府大・工）堀史説、堀達朗、東海旭宏、仲西穂高、岩瀬彰宏	
 	
 (京大・原子炉)坂本雅昭	
 
98

㏻ᖖ᥇ᢥ

CO1-4The Role of Human Oxidation Resistance 1 (OXR1) in Cellular Response to Radiation

A. Matsui, Y. Yoshikawa, A. Yamasaki, T. Saito1, N.
Fujii1, K. Tano1, Q. Zhang-Akiyama

Cell cycle analysis
Nuclei were stained with 50 ug/mL PI. The samples
were analized with FACS.
Targeted disruption of OXR1 in DT40 cells
We prepared chicken OXR1 disrubtion constructs using
puromycin, blasticidin or histidinol resistance gene. The
chicken B lymphoma cells DT40 are cultured andtransfected with the three gene disruption constructs.

Graduate School of Science, Kyoto University
Research Reactor Institute, Kyoto University

1

INTRODUCTION:OXR1 (oxidation resistance 1) isa gene highly conserved in eukaryotes. Previous studies
showed that human OXR1 suppressed spontaneous
mutation in E. coli mutH nth [1]. OXR1 is induced byoxidative stresses such as H2O2 and is localized tomitochondria [2]. However, the function of OXR1
remains to be elucidated. Reactive oxygen species (ROS)
act as a mediator of ionizing radiation -induced cellular
damage. To clarify the protective functions of OXR1
against oxidative damage, we studied the effects of
OXR1 on radiation -generated damage. In this study, weused gamma -ray and high LET heavy -ion beams, which
are known of stronger cell killing effect than X -rays (3).
Our studies showed that OXR1 proteins in HeLa cells
were induced by carbon -ion beam, and that OXR1knockdown HeLa cells were highly sensitive to heavy-ion beams. This year, we found higher micronucleus
formation rate in the cells after irradiation. Then, thecells were released from cell cycle check point earlier
than control cells. To study the function of OXR1 further,
we are now under constructing OXR1-knockout DT40
cells.

RESULTS: The chicken OXR1 targeting constructs,
OXR1-pur, OXR1-bsr and OXR1-his were generated.
DT40 cells are now transfected with electroplation
method. OXR1 -knockout DT40 cells are not gained.
FUTUREPERSPECTIVE:
We
will
try
constructing OXR1 -knockout TD40 cells. After
finishing the step, we will study radation–induced ROS, DNA damages and cell death ofthe construcded cells.

（a）BglII%↓
2%kb%
5’%arm4%kb
XbaI%!
0.8%kb

PvuII!

EcoRI%!

EXPERIMENTS:
Irradiation
HeLa cells stably expressing shRNA targeting OXR1 or
luciferase were synchronized at G1/S phase, andirradiated with gamma -ray (0.77 Gy/min), carbon -ion
(290MeV/nucleon,
87.0keV/um)
or
iron
-ion
(500MeV/nucleon, 64.83 mmH2O) beams generated
by the Heavy Ion Mediacl Accelerator in Chiba(HIMAC). The irradiated cells were incubated（ b）% Puro(3%kb)%%or%%Bsr(4%kb)%%%%%%%%or%His%(5kb)%%

3.13 + cassette kb

BglII%!

3’%arm
1%kb

NotI

5’ arm + pSTBlue-1 + 3’arm = 9kb

3.597 kb

SalI

Fig. 1. (a) Schematic representation of the OXR1 disruption
constructs. (b) Electrophoresis of three constructs.

REFERENCES:[1] M.R. Volkert et al., Proc. Natl. Acad. Sci., (2000)
97, 14530-14535.
[2] N.A. Elliott, M.R. Volkert, Mol. Cell Biol., (2004) 24,
3180-318.
[3] M. Suzuki et al., Int. J. Radiat. Oncol. Biol. Phys.,(2000) 48, 241–250

for about 24 or 34 h, and fixed. The cells wereused in the following experiments.
Micronucleus formation
The nuclei were counter -stained with DAPI.
The
micronuclei
were
detectedwithfluorescence microscopy.

通常採択
採択課題番号 260 1 8
酸化ストレス誘導性タンパク質 OX R1 の機能解析
共同通常（京大院・理）秋山 秋梅、松井 亜子、吉川 幸宏、山崎 晃 (京大・原子炉)田野 恵三、
齊藤 毅、藤井 紀子

99CO1-5Development of an Advanced Optical Fiber Type Neutron Detector

K. Watanabe, Y. Kumagai, A. Uritani, A. Yamazaki,
Y. Sakurai1 and H. Tanaka1

Reactor (KUR). One of the reasons of decrease of thepeak pulse height is expected to be reduction of thetransmittance of the optical fiber. We, therefore, irradiated neutrons to the optical fiber used in our detector.
The neutron flux was 109 n/cm2/s. We continuously
measured the transmittance of the optical fiber by using aspectrometer during the neutron irradiation. The transmittance of the fiber T(t) decreases as;

Graduate School of Engineering, Nagoya University
1
Research Reactor Institute, Kyoto University
INTRODUCTION:
The Boron Neutron Capture
Therapy (BNCT) has been developed as one of thepromising radiotherapies. In this radiotherapy, the neutron dose evaluation is quite important. Therefore, weare developing a novel small neutron flux monitor using
an optical fiber. A small size optical fiber type neutron
detector is one of the promising candidates of the on-line
small neutron flux monitors in BNCT. The conventional optical fiber neutron detectors, however, show no peak
shape corresponding to the neutron absorption reactions,in a pulse height spectrum due to the non-uniform and/or
poor light collection [1-3]. These conventional detectors used ZnS-LiF, Li glass or plastic scintillators. On
the other hand, we apply a new neutron scintillator
Eu:LiCaAlF6. This scintillator has some excellent
properties, such as high light yield, high lithium content,transparency and chemical stability. The light yield of
this scintillator is approximately 5 times higher than thatof the Li glass.
Figure 1 shows the conceptual drawing of the small
size optical fiber type neutron detector. Features of ourdetector are use of a bright scintillator and a quite small
scintillator size. The scintillator size is controlled larger
than ranges of 6Li(n,t) reaction products and smaller than
ranges of fast electrons induced by gamma rays to suppress the signal pulse height only for gamma-ray induced
events.

T t   T0 exp  t /  
where T0; initial transmittance, ; life time of the opticalfiber. We can determine the lifetime by fitting thisequation to the experimental data of decrease of the optical fiber transmittance. Figure 2 shows the wavelength dependence of the lifetime of the optical fiber under neutron irradiation with 109 n/cm2/s. The lifetime ininfrared region is confirmed to be longer than that in ultraviolet and visible region. The emission wavelengthof the Eu:LiCaAlF6 scintillator is 380 nm, where the lifetime of the transmittance is not so long. From theseresults, one of the reasons of decrease of the peak pulse
height is confirmed to be reduction of the transmittanceof the optical fiber.

-1
減衰定数(s)Lifetime (s)107

HV
Optical fiber

PMT

MCA

400

500

600

700

800

波長(nm)
Wavelength
(nm)

Amp.

Fig. 2PC

Fig. 1

105
104
300

Preampscintillator

106

Wavelength dependence of the lifetime under
neutron irradiation.

In infrared region, the neutron radiation hardness isquite high. If we can use a neutron scintillator with
infrared emission, the radiation hardness of the opticalfiber type neutron detector can be improved.

Conceptual drawing of the optical fiber typeneutron detector.

So far, we evaluated dynamic range and long term stability of our detector. Our detector was confirmed toshow good linearity up to 109 n/cm2/s. However, peakpulse height decreases due to neutron irradiation. In
this report, we experimentally evaluate neutron radiation
hardness of the developed detector.
RADIATION HARDNESS TEST: We fabricated theoptical fiber type neutron detector using a small
Eu:LiCaAlF6 scintillator and experimentally evaluated its
radiation hardness at the Heavy Water Neutron Irradiation Facility (HWNIF) of Kyoto University Research

REFERENCES:[1] M. Ishikawa et al., Appl. Rad. Isotopes, 61 (2004)
775-779.
[2] M. Ishikawa et al., Nucl. Instr. Meth. A, 551 (2005)
448-457.
[3] Y. Ito et al., Radiat. Prot. Dosim., 110 (2004)
619-622.

採択課題番号 26021 極小検出器を用いた中性子計測手法の高度化に関する研究
共同通常
通常採択
（名大・工）瓜谷章、渡辺賢一、山﨑淳、熊谷洋祐 （京大・原子炉）櫻井良憲、田中浩基
100CO1-6Focusing Test of an Ellipsoidal Neutron Mirror with a Metal Substrate

M. Hino1, J. Guo2, S. Takeda3, T. Oda1, S. Morita2*,
J. Kato2, Y. Yamagata2, M. Furusaka3, Y. Kawabata1
1
Research Reactor Institute, Kyoto Univ., Japan
2
RAP, RIKEN, Japan,
3
Grad. Sch. of Eng., Hokkaido Univ., Japan*
Present address: Tokyo Denki Univ. Japanneutrons without supermirror coating.
EXPERIMENTS: The design, manufacturing andpolishing of the mirror were carried out by RIKEN [1].
The form accuracy of the mirror was estimated to be
5.3 μm Peak-to-Valley (P-V) and 0.8 μm P-V for theminor-axis and major-axis direction respectively,
while the surface roughness was reduced to 0.2 nm
rms. The neutron focusing performance of the mirror
was evaluated using CN3 beam line at Kyoto
University Research Reactor (KUR-CN3).
RESULTS: As shown in Fig.1, the two-dimensional(2D) image of neutron beam reflected by an ellipsoid
focusing mirror was clearly changed as a function of
distance between the mirror center and detector.
Cadmium (Cd) pinhole with an aperture size of 1 mm
in diameter to choose incident beams from the CN3
guide a Cd U-shape slit to remove unnecessary
neutron beams affecting the focusing. The circularfocusing spot at the focal point was almost equivalent
to that of the pinhole.
REFERENCES:[1] J.Guo, et al., Optics Express,
22(2014)24666-24677.

INTRODUCTION: Progress of neutron opticaldevices is significant, however, it is still very difficult
for neutron aspherical focusing mirror. Because therequired surface roughness is smaller than 0.5 nm
even for m=3 supermirror coating and the mirror sizeis large. In order to realize large ellipsoid neutron
focusing mirror, we are doing several trials. In thisstudy, we show the neutron focusing experimental
result of ellipsoid mirror with a metal substrate. In
general it is very difficult to make a smooth surface on
metal due to the grain structure. By using electrolessnickel-phosphorus (NiP) plated material, we canovercome this problem. Electroless NiP has great
advantages for realizing neutron mirror because of its
amorphous structure, good machinability andrelatively large critical angle of total reflection for

Fig.1 Schematic layout of neutron focusing experiment at KUR-CN3 and the 2D images of beam shapes as a functionof the mirror center to detector distance (MDD), and the direct beam shape without the focusing mirror at the focal
point.

採択課題番号 26065
次期中性子ビーム科学施設のための中性子光学デバイス開発 共同通常
通常採択
Fig.2 Measured reflectivity of the m=5 flexible NiC/Ti supermirror sheet bounded on flat plate.
（京大・原子炉）日野正裕、小田達郎、川端祐司 （KEK・IMSS）山田悟史、遠藤仁、瀬戸秀紀（理研）郭江、森田晋也、加藤純一、山形豊 （北大）武田晋101

CO1-7

Examination of the Usefulness as the New Boron Compound of KA-BSH
for Born Neutron Capture Therapy

Gen Futamura1, Shinji Kawabata1,
Shin-Ichi Miyatake2, Toshihiko Kuroiwa1,
Yoshihide Hattori4, Mitsunori Kirihata4, Hiroki Tanaka3,
Yoshinori Sakurai3, Shin-Ichiro Masunaga3, Koji Ono3

travenous administration (iv) and neutron irradiated;
Group 2, KA-BSH administered by convection enhanced
delivery (CED) by using Alzet pump, which can deliver
solutions directly into the solid tissue with continuouspressure gradient distribution [2, 3], and neutron irradiated; Group 3, neutron irradiation; Group 4, untreatedcontrols. BNCT was initiated 1 h after termination of
Alzet pump infusion or i.v. administration. All irradiated rats were anesthetized with a pentobarbital sodium.
The rats were irradiated for 60 min with 1MW. The
antitumor effects of BNCT were evaluated in the mean
survival times (MSTs) of the rat.

1

Department of Neurosurgery, Osaka Medical College
Division for Advanced Medical Development, Cancer
Center, Osaka Medical College
3
Research Reactor Institute, Kyoto University
4
Osaka Prefecture University

2

INTRODUCTION:
Boron neutron capture therapy (BNCT) is an attractive
technique for malignant brain tumor treatment. [1] It is
important to have a significant differential uptake of 10B
between tumor cells and normal cells to achieve potent
tumor-selective antitumor effects.
Today, clinicallyused dodecaboranethiol (BSH) is transferred to brain tumors only through the disrupted blood-brain barrier(BBB), so it is difficult for BSH to reach regions thattumor cells invade microscopically where the BBB seems
to be normal. On the other hand, boronophenylalanine(BPA), which transfers boron via L-type amino acidtransporter, can deliver 10B even in the infiltrating tumor
cell population where the BBB is normal. However,some amounts of 10B are inevitably taken into the normal
cells by BPA systemic administration. A wide variety ofboron delivery agents have been synthesized to solvethese problems. [1] Kojic acid (KA) was reported as theagent which showed intense uptake in malignamt tumor.
Therefore, we designed and synthesized KA-BSH andevaluated therapeutic effect of KA-BSH as boron delivery agents for BNCT in F98 glioma cell bearing rat brain
tumor model.

RESULTS:The estimated physical radiation doses delivered to tumor,
brain and blood were calculated according to boron concentrations. The physical radiation doses delivered tothe tumor were 1.1Gy for KA-BSH administered by iv.
The corresponding normal brain doses were 1.0Gy. The
survival data of Group 1, 2, 3 and 4 following BNCT
showed that the MSTs were 35.4±8.0 days, 29.8±3.3 days,
30.2±2.2 days and 28.5±3.1 days, respectively.
We accepted significantly extend the duration of survival
time of the rats group using KA-BSH administered by iv(Group 1), compared with the neutron irradiation only
(Group 3) (p<0.005).

CONCLUSION:
Survival times of group1 were significantly prolonged
even compared with irradiation group. The therapeutic
effect of KA-BSH administered by iv was higher thanthat we expected from these tissue boron concentrations
and physical radiation doses. This study suggested that
KA-BSH might have extremely high compound biological effectiveness (CBE), and KA-BSH might be the drug
to add therapeutic effect of clinical BNCT using BPA orin combination with BPA / BSH to.

MATERIALS AND METHODS:
BNCT was performed 14 days following stereotactic implantation of 103 F98 glioma cells implanted rat brain
tumor model. Rats were transported to the Nuclear Reactor Laboratory at Kyoto University Research Reactor
Institute.
Based on the results of the biodistribution study, we prepared 4 groups. The rats were then randomized on thebasis of weight into experimental groups of 6-8 animals
each as follows: Group 1, KA-BSH administered by in-

REFERENCES:[1] Barth RF et al: Radiat Oncol 7: 146, 2012.
[2] Hiramatsu R et al: J Pharm Sci 104: 962-70, 2015
[3] Kawabata S et al: J Neurooncol 103: 175-85, 2011

採択課題番号 26078
新規硼素化合物の有用性と腫瘍幹細胞の克服
通常採択（大阪医大）黒岩敏彦、宮武伸一、川端信司、二村元、東保太一郎、木村誠吾、大村直己（岡山大）道上宏之（京大原子炉）増永慎一郎、小野公二
102

CO2-1 Development of Measurement Method for Epi-Thermal Neutrons Using the 10B(n,)Reaction
T. Matsumoto, A. Masuda, H. Harano, H. Tomita1, K. Ito1,
Y. Ichinose1, J. Kawarabayashi1, T. Iguchi1, K. Watanabe1,
A. Uritani1, J. Hori2, Y. Sakurai2

The detection system were experimentally tested using
the neutron beam from a neutron source with the photo
neutron reaction by means of the TOF method. Fig.1
shows the pulse height spectra of the NaI(Tl) scintillator
with and without the coincidence measurements. In the
NaI(Tl) scintillator, 478 keV gamma rays due to the10
B(n,) reaction is detected around 600 channel. The
counts due to other gamma rays by the coincidence
measurements. In the experimental room, many boron isused in shielding materials and collimators. Background measurements with only NaI(Tl) detector werealso performed.
Characteristics of a prototype of epithermal neutron imaging camera were also measured using the TOF method.
The prototype detector consists of a silver plate as a resonance filter, a B4C thermal neutron absorber, and a
GEM with a neutron converter of 10B.
RESULTS: From the coincidence measurement, countrates for the LGB detector (N)) and the NaI(Tl) detector(N) and coincidence count rate (N) are derived. Neutron capture reaction rate due to the 10B(n,) reaction isderived from NN/N. Neutron fluence was finally determined using ratio of count rates in measurements withand without the thick natB total absorption sample. The
experimental results are checked by Monte Carlo simulations in future.

National Metrology Insitute of Japan, National Instituteof Advanced Industrial Science and Technology
1
Department of Engineering, Nagoya University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: Evaluation of neutron dose equivalent for the epi-thermal neutron region is very importantin work places with neutron sources or nuclear fuels aswell as irradiation fields in a boron neutron capture therapy. A new calibration method for the response of neutron dosimeters has been developed using a pulse white
neutron beam[1]. On the other hand, it is not easy tomeasure precisely the neutron fluence for epi-thermal
neutrons in an irradiation field, although a gold activation
method is usually used in a thermal neutron region, andan elastic neutron scattering reaction with hydrogen atoms is adopted in a fast neutron region to measure precise neutron fluence. In the present study, we have developed a measurement method for epi-thermal neutrons
using a 6Li6natGd10B3O9:Ce+ (LGB) and an NaI(Tl) scintillators. We also developed an epi-thermal neutron camera consisting of GEMs and resonance filters for neutrons
up to 10 keV.
EXPERIMENTS: A collimated neutron beam throughcollimators was obtained by the photo neutron reaction
using a water-cooled tantalum target at the KURRI Linac[2]. The 50 mm-diameter and 5-mm thick LGB scintillator was set at the center of the neutron beam. The
76.2 mm-diameter and 76.2 mm thick NaI(Tl) was located out of neutron beam at an angle of 135 degrees withrespect to the neutron beam direction. When the LGB
scintillator detects neutrons by the 10B(n,) reaction,
478 keV monoenergetic gamma rays are produced andsubsequently detected with the NaI(Tl) scintillator. In
the coincidence measurements, the neutron capture reaction rate in the LGB scintillator is obtained without detection efficiencies of the LGB and the NaI(Tl) scintillators. Moreover, the absolute neutron fluence is determined by measuring gamma rays from the 10B(n,) reaction with the NaI(Tl) scintillator in setting a 5-cm thicknat
B total absorption sample in front of the LGB scintillator.

Counts/Channel

104
478 keV  ray

103

Net PH (N)

102
101
100

Coincidence PH
0

1000
2000
NaI(Tl) Pulse Height Channel

Fig.1. Pulse height spectra measured with the NaI(Tl)detector.
REFERENCES:[1] T. Masumoto et al., KEK proc. 2011 (8), 218-225(2012).
[2] K. Kobayashi et al., Annu. Rep. Res. Reactorinst. Kyoto Univ. 22, 142 (1989).

採択課題番号 26055 熱中性子フルエンス率の測定の高度化とその国際標準化に関する研究共同通常
通常採択（産総研）原野英樹、松本哲郎、増田明彦、（名大）井口哲夫、瓜谷章、河原林順、渡辺賢一、富田英生、伊藤海、一之瀬裕一郎、杉本大（京大・原子炉）堀順一、櫻井良憲
103CO2-2

Measurement of Gamma Ray and Neutron Spectrum of Curium Isotope (3)Y. Nauchi, J. Hori1, T. Sano1

rates are compared in Table 2. Considering the differenceof neutron spectra shown in Fig 3, the count rates in thetwo detectors agree fairly well (18% difference inCM244). Accordingly, absolute measurement of neutrons
from the sample would be capable for CM samples taking
the neutron spectrum into account.
REFERENCES:[1] T. Fujii et al., Conf. Record 2010 Annual Meeting of
AESJ pp58-66 (on CD-ROM).
[2] A. G. Seamster et al., Phys. Rev. C 29 (1984) 394
Table 1: Isotopic composition of Cm samples [1]Central Research Institute of Electric Power Industry
Research Reactor Institute, Kyoto University

1

244

Sample

245

Cm

246

Cm

Cm

CM244

88.53

3.13

8.34

CM246

24.18

1.11

62.18

247

Cm

248

3.00

Cm

9.53
CM244
CM246

gamma ray spectra (cps/MeV)

208Tl
100

4.82MeV102.235MeV
2.61MeV
2.98MeV 3.04MeV
1

3.04MeV
3.79MeV
2

2.5

3

3.5
Energy(MeV)

4

4.5

5

Fig. 1  ray spectrum measured for CM244 and CM246 .
gamma ray spectra (cps/MeV)

1000

CM244 behind Poly.
CM246 behind Poly.
CM244 No Poly

H(n,) Al(,)
100

10

1
2.15

2.2

2.25
Energy (MeV)

2.3

2.35

Fig. 2 H(n,) spectrum overlapped by Al(,) spectrum
Pulse height spectrum (cps/MeV)INTRODUCTION: Yields and spectra data of neutrons and higher energy (>3MeV)  rays from thespontaneous fission of 244Cm has been focused on since
they are major source in spent nuclear fuel. The radiations would be significant indicators of existence of nuclear materials. However those measured data are scarce.
KURRI have possessed Cm samples (Table 1 [1]) in
which Cm2O3 are diluted in aluminum (Al) powder encapsulated in Al cladding. In this work, preliminary
characterizations of CM244 and CM246 are done.
GAMMA RAY MEASUREMENTS:  rays from samples were measured with a Ge detector of 20%
effeiciency.  rays radiated subsequent to  decays were
measured. For CM244 and CM246 samples, multiple rays of different energies from 243, 244, 245Cm were wellmeasured. The activity ratio of CM244/CM246 are
0.935± 0.0191 and 0.714±0.004 for 244,245Cm, respectively. The ratios agree with the data in Table 1.
Then, higher energy  rays from 2 to 5MeV are focusedon to clarify whether noise spectra exist or not for measurements of 2.223MeV and fission  rays. As shown in
Fig. 1 and broader peaks from 2.5 to 5MeV are found forCM244. The bump spectra exist only slightly for CM246
so it is considered the fission  ray spectrum dominates
the energy region above 2.3MeV in CM246. The resolutions of the peaks are poorer than 2.6145MeV  ray from208
Tl. That indicates the  rays are radiated from compound nucleus moving with a certain kinetic energy morethan keV. Based on literatures, the 2.235MeV  rays
might be attributed to 27Al(,) reactions [2]. The originof the other higher energy  rays are unknown althoughneutron direct interactions with Ge detertor materials are
not the candidates since such bump spectra were notfound for a case when 252Cf was put alternatively to CM
samples.
The higher energy bumps should be eliminated to quantify fission  ray spectrum. For the purpose with the samples, coincidence measurements with multiple detectors
would be required as well as studies on nuclear physics to
explore the reactions radiating such  rays.
NEUTRON MEASUREMENTS: By putting CM samples and Californium (252Cf) neutron source behind polyethylene block of 10cm thickness, the H(n,) 2.223MeV 
rays were measured with the Ge detector. As shown in
Fig. 2, 2.235MeV  ray spectrum overlaps the 2.223MeV
one for CM samples. The former was subtracted from thelatter by normalizing the count rate of the former over a
region from 2.235 to 2.250MeV to that of latter. Then the
count rate of the 2.223MeV  rays was estimated. On theother hand, fast neutrons from the CM samples were
measured with a NE213 scintillator. The measured count

101

CM244
CM246
Cf252

100
10-1
10-2
10-3
0

1

2
3
4
5
6
Pulse height (MeV-electron equivalent)

78Fig. 3 Neutron spectrum measured with NE213.
Table 2: Count rate ratio of neutrons for CM / 252Cf
MethodCM244/252Cf

rel.err

CM246/252Cf

H(n,γ)

0.212

0.030

0.860

0.019

NE213

0.180

0.063

0.843

0.012

採択課題番号 26057 キュリウム核種のガンマ線と中性子発生スペクトルの測定(3)（電中研）名内泰志（京大・原子炉）堀順一、佐野忠史
104

rel.err

通常採択

CO2-3 Development of Hybrid Ce:LiCAF Scintillator for Nuclear Data Measurement
T. Fujiwara1,4, D. Matsuyama2, K. Tagi2, Y. Kusumawati2,
J. Hori3, T. Sano3, and M. Uesaka1

excellent performance for high energy neutron measurement. 8 m TOF line at KURRI.
In addition, low gamma-ray sensitivity great gamma/neutron discrimination with pulse height and showedvery quick recovery from gamma-burst which enableshigh energy neutron measurement.

1

Nuclear Professional School, The University of Tokyo
Department of Nuclear Engineering and Management,
The University of Tokyo
3
Research Reactor Institute, Kyoto University
4
National Metrology Institute of Japan, National Instituteof Advanced Industrial Science and Technology
2

INTRODUCTION: Precise nuclear data measurement
is needed for new generation reactor design and development. In this field, neutron Time-of-Flight (TOF)
measurement with pulsed neutron source is playing important role.
In this work, we report on the first nuclear data measurement at KURRI-Linac neutron source with hybrid
Ce:LiCAF scintillator which has high neutron detection
efficiency and better gamma-ray discrimination[1][2].
Ce:LiCAF covered with plastic scintillator[3] showed excellent characteristics in the detection efficiency andgamma-ray discrimination compared with other conventional scintillators, such as Li-Glass and Li:ZnS scintillators. Especially, excellent pulse height discrimination ofneutrons from gamma rays and very short decay time arevery promising for a new field of fast neutron detection
and great recovery from the gamma-flash.

Fig. 1. Pulsed height spectrum of Ce:LiCAF based
hybrid scintillation neutron detector. Showed clear neutron peak and low sensitivity to gamma-ray.

EXPERIMENTS: Neutron transmission experiments(NRTA: Neutron Resonance Transmission) were carriedout at 8m TOF line at KURRI-Linac. 237Np sample wasplaced at the neutron beam line, and the detector wereplace in 50 cm behind the sample.
Accelerator was operated in 50Hz and 100ns pulse
width. We have fabricated hybrid scintillator based on 10
×10 × 2mm size Ce:LiCAF scintillator crystal. The crystal were covered with plastic scintillator (PPO and
POPOP) and coupled to photo multiplier tube (Hamamtsu
R329-05). 5mm thick Pb filter was placed to reduce
gamma-rays. Fast Comtec MPA3 were used for DAQ
system.

Fig. 2. First result of neutron transmission experiment(NRTA: Neutron Resonance Transmission) of 237Np.
The measurement were carried out at 8m TOF line at
KURRI-Linac

RESULTS: Fig. 1 shows pulse height spectrum ofneutron detector. The line in green shows energy spectrum of neutron and gamma-ray mixed field, and the lingin pink represents a energy spectrum when neutron wereshielded with Boron. As shown in Fig. 1, clear neutron
peak and very low sensitivity to gamma-ray were observed, which stands for great gamma-ray discrimination.
This is due to coupling Ce:LiCAF scintillator with plastic
scintillator which enables to improve alpha/beta ratio.
With our detector, we successfully measured high energy
neutrons up to 2.4 keV. Fig. 2 shows the absorption neutron cross-section of 237Np.
We conclude that TOF spectrum of Ce:LiCAF showed

REFERENCES:[1] A. Yamazaki et al., Nucl. Instr. and Meth. A (2011),
doi:10.1016/j.nima.2011.02.064[2] K.Watanabe et al., Conference record of NSS IEEE,
201[3] T. Fujiwara et al., Neutron News, vol. 23, no. 4, pp.
31–34, Nov. 2012.

<;NTG0  UP"!$!E'A,?$ $"MKRH 通常採択
V=5#7DJIWL/ * V=5#7W>6 5@F+ 2B
    &3 - V(
5#(5CW4 S%)Q :9

105

CO2-4

Investigation of Variable Neutron Field for Accurate Determination of
Thermal Neutron Capture Cross Section at KURRI-LINAC

J. Hori, T. Yagi, T. Sano, Y. Takahashi, H. Yashima

ured TOF spectra and the evaluated neutron capture crosssections of JENDL-4.0 [2] as listed in Table 2. The calculated reaction rates were in agreement with the experimental ones within 2 % accuracy. As a result, it was confirmed that the neutron spectrum information obtained by
the TOF method can be used for activation analysis.
In nearly future, we will apply the spectrum determination method to the activation experiments for MA.

Research Reactor Institute, Kyoto University

In order to reduce radioactive
toxicity, feasibility for nuclear transmutation of minor
actinides (MAs) and long-lived fission products(LLFPs) by utilizing innovative nuclear system has
been investigated. The report on OECD/NEA No.6410[1] indicates that there are large gaps on capture crosssections of minor actinides (MAs) between current
uncertainty and required accuracy.
Since high-intensity-pulsed neutron sources withspallation reaction such as CERN, LANL and J-PARC
become available, statistical error of relative neutron
capture cross sections of MAs with time-of-flight(TOF) method was decreasing drastically. However,accurate normalization of TOF data is still an important issue, and unrecognized bias effect needs to beeliminated as much as possible. In this study, we proposed the thermal capture cross section measurement
methods using variable neutron fields and developed
variable neutron fields in the KURRI-LINAC.
INTRODUCTION:

Table 1 Boric-acid concentration of the light water moderator

EXPERIMENTS: In order to cross checked the neutron capture cross sections by integral measurements
using variable neutron flux field, KURRI-LINAC
based neuron source was utilized. Neutrons producedby photonuclear reactions were moderated by lightwater. Four kinds of variable neutron flux fields wereconstructed by merging boric-acid solution into thelight water moderator, as listed in Table. 1. Neutron
spectra of these fields were obtained by TOF measurement of the capture gamma-rays from the 10B(n,)reaction with twelve Bi4Ge3O12 (BGO) scintillators,
which located at 12.7±0.02 m from the photoneutron
source. The linac was operated with a repetition rate of
50 Hz, a pulse width of 100 ns, an averaged current
was 18 A and an electron energy of about 30 MeV.
Gold foils with and without Cd cover were also irradiated for each moderator. Reaction rates were obtainedwith an activation foil method.

Fig. 1 Neutron spectra for moderators with different
boric-acid concentration measured by TOF
methodTable 2 Comparison of normalized reaction rates of
197
Au(n,)198Au

Present study includes the results 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 and Technology of Japan (MEXT).

RESULTS: Figure 1 shows the neutron spectra formoderators with different boric-acid concentration measured by the TOF method. The thermal bumps were fittedwith the Maxwell distribution and the neutron temperatures were determined from 319.5 to 430.8 K. On theother hands, the reaction rates of 197Au(n,)198Au derived
from the activation method experimentally were compared with the calculated reaction rates using the meas-

REFERENCES:[1] M. Salvatores et al., WPEC-26, OECD NEA (2008).
[2] K. Shibata et al., J. Nucl. Sci. Technol. 48(1) (2011) 1-30.

採択課題番号 26069
長寿命放射性核種の中性子核データ精度向上に係る研究開発（京大・原子炉）堀 順一、佐野 忠史、高橋 佳之、八島 浩
106

通常採択

CO2-5Experimental Study on Non-destructive Assay with a Pulsed Neutron Source
RESULTS: The TOF spectra for the mixture composedof natU, 237Np and 243Am are shown in Figs. 1 and 2. Although many resonance dips from the impurities of 237Np
and 243Am were observed (Fig. 1), there are no differences between TOF spectra with only natU (blue line) andthe mixture (red line) (Fig. 2). This result indicates thatthe self-indication TOF spectrum was not greatly influenced by nuclide impurity. It was experimentally shownthat the contribution from the other nuclide can be remarkably suppressed by applying the self-indication
method.

J. Hori, T. Sano, Y. Takahashi, H. Unesaki
and K. Nakajima
Research Reactor Institute, Kyoto University
INTRODUCTION: Non-destructive assay of nuclear
fuel materials in spent nuclear fuel is a key technology
for nuclear material accountancy and critical safety. Neutron Resonance Densitometry (NRD) with a pulsed neutron source has been developed for a non-destructive assay of material [1]. In this method, we can identify andquantify the target nuclide by measuring the neutron resonance absorption with the Time-of-Flight (TOF) technique. There are two ways to measure the neutron resonance absorption. One is Neutron Resonance Transmission Analysis (NRTA) [2] and another is Neutron Resonance Capture Analysis (NRCA) [3, 4].
In this work, we have proposed a new concept of“self-indication method” combined with NRTA and
NRCA. In the self-indication method, we set an indicatorconsisted of target nuclide with a high purity at thebeam-downstream from a sample. By detecting the reaction products such as neutron capture  rays or fission
products from the indicator with the TOF method, thetransmission neutron can be measured indirectly. The
self-indicator is a transmission neutron detector which
has a high efficiency around the objective neutron resonance energies of target nuclide, so that it enables us toquantify effectively the amount of resonance absorptionof the target nuclide. Moreover, it is hard to be affectedby the decayed -rays from the fuel.

Fig. 1 TOF spectra obtained with NRTA for natU and mixtureof natU, 237Np and 243Am

EXPERIMENTS: We demonstrated a nondestructive
assay for nuclear material using a 46-MeV electron linear
accelerator at the Kyoto University Research Reactor
Institute. A mixture sample of a natural uranium plate andsealed minor actinides such as 237Np and 243Am was used
as a sample. The natural uranium plate was 10×20 mm2
and weighted 5.8 g. The samples of 237Np and 243Am
were oxide powder, which was pressed into a pellet 20mm in diameter and encapsulated in an aluminum
disk-shaped container 30 mm in diameter with
0.5-mm-thick walls. The activities of 237Np and 243Am
were 26 and 868 MBq, respectively. The 10B plug 8 mm
thick or a natural uranium plate of 10×20 mm2 andweighted 5.8 g was used as an indicator. Prompt-capture
-rays from the indicator were measured with a pair of
Bi4Ge3O12(BGO) detectors in the TOF experiment. Since
the 10B indicator can absorb most neutrons with energies
below the epithermal-region, it was equivalent to theconventional NRTA. In the latter case, it was theself-indication measurement.

Fig. 2 TOF spectra obtained with the self-indication method
for natU and mixture of natU, 237Np and 243Am

This work was supported by JSPS KAKENHI Grant
Number 24760714.
REFERENCES:[1] H. Postma et al., Radioanalytical and Nucl. Chemistry,
248, (2001) 115-120.
[2] J. W. Behrens et al., Nucl. Technol., 67, (1984)
162-168.
[3] Y. Kiyanagi et al., J. Nucl. Sci. Technol., 42, (2005)
263-266.
[4] A. Pietropaolo et al., Applied Spectroscopy, 64,(2010) 1068-1071.

採択課題番号 26070

パルス中性子源を用いた核燃料物質の非破壊定量及び可視化技術の開発（京大・原子炉）堀 順一、高橋 佳之、佐野 忠史、中島 健、宇根崎 博信
107

通常採択

CO3-1Development of In-reactor Observation System Using Cherenkov Light (VI)

T. Takeuchi, K. Yamamoto, N. Otsuka, H. Shibata,A. Shibata, N. Takemoto, K. Tsuchiya, T. Sano1,
H. Unesaki1, Y. Fujihara1, Y. Takahashi1
and K. Nakajima1

the change rates of the brightness are larger and smaller
than that of the total output power, respectively. The difference in the change rate between the TC and D2O sides
is thought to be due to an inhomogeneous distribution of
output power, resulting in the difference in the amount of
the Cherenkov light. On the other hand, the absolute value of the brightness of the TC side was smaller than thatof the D2O side at from 1 to 2 MW. A possible explanation is that the shadow of the control-rod guide tubes andthe other irradiation equipment were included in image of
the CCD camera. To suppress the effect of the shadow on
the analyses of the brightness, the observations of theCherenkov light from various positions using a numberof cameras might be required.

Neutron Irradiation and Testing Reactor Center, JAEA
1
Research Reactor Institute, Kyoto University
INTRODUCTION: The surveillance system which
can visualize and quantitatively evaluate reactor statuses
will contribute to reactor operation management. We
started the development of the on-line reactor core imaging system using Cherenkov light[1] in 2009. Previously,
the total reactor power of the KUR can be estimated using the CCD camera by the method of dissolving the total
image brightness to the RGB brightness components[2]. In
this study, the correlation between the reactor power andthe image brightness of the Cherenkov light from a specific fuel element was evaluated in an effort to evaluate
the output power of each fuel element.

CONCLUSION: As part of the development of thevisible on-line core surveillance system, the Cherenkov
light at the core of KUR observed by a CCD camera wasanalyzed on the correlation between the image brightnessof the Cherenkov light and the output power about a specific fuel element. The results indicate that the inhomogeneous distribution of output power and the shadow of
the control-rod guide tubes and the other irradiationequipment have significant effects on the brightness of
the Cherenkov light. These effects could be suppressedby using a number of cameras located at various positions.

EXPERIMENTS: The CCD camera (AEC-100ZL, Q·I
Inc.) was inserted into core-observation pipe of KUR
during increasing the reactor power from 1 to 5 MW. The
output of the CCD camera was collected by an image
recorder. The Cherenkov light from the target fuel element shown in fig. 1 was analyzed. The brightness signalof the output image from the CCD was dissolved to RGB
color signals (R:700nm, G:546.1nm, B:435.8nm)[3]. The
R component without halation was used to correct the
total image brightness.

REFERENCES:[1] J.V. Jellry, Cherenkov Radiation and its Applications(Pergamon, New York, 1958).
[2] N. Otsuka, et al., KURRI Progress Report, (2013) P.
215.
[3] Commission internationale de l'Eclairage proceedings,
1931, Cambridge.

RESULTS: Figure 2 shows the results of the analysesof the Cherenkov light from the TC and D2O sides of thetarget fuel element. Although the averaged brightnesschanges at an almost same rate as that of the total output
power, at the TC and D2O sides of the fuel element,

TC sideD2O sideFig. 2. The change rate of the brightness of theCherenkov light from the target fuel element withthe reactor power.

Fig. 1. The array of the fuel elements at the core of
KUR. The red boxed fuel is the target one. The blackband at the middle of the fuel element is the handle.

採択課題番号 26040 チェレンコフ光を用いた試験研究炉の炉内監視手法の研究開発 通常採択
（原子力機構）土谷邦彦、武内伴照、大塚紀彰、柴田裕司、柴田 晃、山本圭一、竹本紀之（京大・原子炉）中島 健、宇根崎博信、佐野忠史、藤原靖幸、高橋佳之
108CO3-2 Neutron Irradiation Effect of High-density MoO3 Pellets for Mo-99 Production (2)After the dissolution of irradiated MoO3 pellets andextraction of 99mTc solution, 99Mo and 99mTc activities
were measured in the Mo solution and 99mTc solution by
the germanium detector. From the result of the -ray
spectrum of Mo solution and 99mTc solution, the ratio of
measured value and calculated value (M/C) was 1.05 andit was confirmed that the calculated 99Mo marched themeasured one within an error of ±5% by the previous
method [3]. On the other hand, 92mNb observed in the
Mo solution as impurities. 92mNb was not measured in
the 99mTc solutions. Table 2 shows the result of 99mTc
recovery rates from the Mo solution. The recovery rateof the 1st and 2nd runs achieved the target values (>80%).
The 3rd and 4th runs were less than 60%. In this experimental, different MEKs were used for the extraction tests
and it seems that the 99mTc recovery rate affected purityof MEK.
Impurities such as Al, Mo and MEK, radiochemical
purity and radionuclidic impurity were measured with the
99m
Tc solution in the 1st run and the high purity 99mTc solution was obtained by this method.

K. Nishikata, T. Ishida, M. Yonekawa, Y. Kato,
M. Kurosawa, A. Kimura, Y. Matsui, K. Tsuchiya,
T. Sano1, Y. Fujihara1, Y. Takahashi1 and J. Zhang1
Neutron Irradiation and Testing Reactor Center, JAEA
1
Research Reactor Institute, Kyoto University
INTRODUCTION: As one of effective applications of
the Japan Materials Testing Reactor (JMTR), JAEA has aplan to produce 99Mo by (n, γ) method ((n, γ)99Mo production), a parent nuclide of 99mTc [1]. In this study, preliminary irradiation test was carried out with thehigh-density molybdenum trioxide (MoO3) pellets in thehydraulic conveyer (HYD) of the Kyoto University Research Reactor (KUR) and the 99mTc solution extracted
from 99Mo was evaluated.
EXPERIMENTS:
The high-density MoO3 pellets
were fabricated by the Plasma Sintering Method [2].
Dimension and density of MoO3 pellets were 18×10 mm
and about 92.5%T.D., respectively. The MoO3 pellets
were irradiated in the HYD of the KUR. Before theirradiation test, neutron flux in the HYD was measured
with the dosimeters (In foil and In-Ni foil with Cd canning). Table 1 shows the irradiation conditions of MoO3
pellets in the HYD. After the irradiation tests, the irradiated MoO3 pellets were transported from KUR to
JMTR-HL. The irradiated pellets were dissolved with
6M-NaOH solution in the Lead Cell and the 99mTc was
extracted from the Mo solution by the solvent extraction
method using methyl ethyl ketone (MEK).

Result of 99mTc recovery rates from the Mo
solution
Activity of 99mTc
Recovery rate
No.
(Bq)
(%)
1st run1.09 × 109
82.3
2nd run8.53 × 108
95.7
rd
3 run
3.09 × 108
56.5
th
8
4 run
2.41 × 10
55.1

Table 2

Table 1 Irradiation conditions of MoO3 pellets
Items
Thermal power

1 MW

Thermal neutron flux

1.82 × 10 ± 4.18 × 1015 m-2s-1

Epithermal neutron flux

7.08 × 1016 ± 2.29 × 1015 m-2s-1

Fast neutron flux

7.13 × 1016 ± 1.85 × 1015 m-2s-1

Irradiation time
Irradiation temperature

CONCLUSION: After the irradiation test of thehigh-density MoO3 pellets in the KUR, 99mTc was extracted from the Mo solution and the recovery rate of99m
Tc achieved the target values. The 99mTc solution
also got the value that satisfied the standard value for99m
Tc radiopharmaceutical products by the solvent extraction method.

Values17

3.2 h

REFERENCES:[1] K. Nishikata, et al., Fabrication and Characterizationof High-Density MoO3 Pellets, Proceedings of 2012
Powder Metallurgy World Congress & Exhibition(2012) CD-ROM.
[2] K. Tsuchiya, et al., Status of 99Mo-99mTc Production
Development by (n, γ) Reaction, JAEA-Conf
2011-003（2011）.
[3] K. Nishikata, et al., Neutron Irradiation Effect ofHigh-density MoO3 pellets for Mo-99 Production,
KURR Progress Report 2013, p242.

below 90°C

RESULTS: After the irradiation test, all of the diffraction peaks corresponding to the orthorhombic crystal
structure (-MoO3) were assigned to MoO3 appeared in
the irradiated MoO3 pellet. The Grain sizes of MoO3 pellet before/after neutron irradiation were almost identical(approx. 1μm). The results suggest that No change ofcrystal structure and grain size was observed in the MoO3
pellets irradiated at low temperature and low fluence.

採択課題番号 26041
高密度 MoO3 ペレットの照射効果に関する研究（JAEA）西方 香緒里、石田 卓也、米川 実、加藤 佳明、黒澤 誠、木村
土谷 邦彦
（京大・原子炉）佐野 忠史、藤原 靖幸、高橋 佳之、張 倹
109

通常採択
明博、松井 義典、

CO4-1Development of Radiation Tolerant Image Sensor
with Field Emitter Array

Y. Gotoh, M. Nagao1, T. Okamoto2, T. Masuzawa3,
Y. Neo3, H. Mimura3, H. Tsuji, M. Akiyoshi, I. Takagi,
N. Sato4

ance against –ray irradiation.

Graduate School of Engineering, Kyoto University
National Institute of Advanced Industrial Science andTechnology
2National Institute of Technology, Kisarazu College
3
Research Institute of Electronics, Shizuoka University
4
Research Reactor Institute, Kyoto University

Current (A)1

INTRODUCTION: One of the most serious problems
for the observation of interior of the nuclear reactor at theElectric Power Plant, Fukushima the 1st, is such that there
are no good cameras that can stand for the irradiationfrom radioactive material can be seen as a commercial
product. Therefore, it is necessary to develop a reliablecamera that can be used under hard radiation. The purpose of the present study is to develop a compact image
sensor for visual light with a field emitter array (FEA).
To ensure the radiation tolerance, it is necessary to show
the resistance of each element against -ray radiation.
Change in the operational characteristics of the key
components of the image sensor, FEA [1] andphotoconducting diode [2] was investigated.

10

−4

10

−6

10

−8

10

−10

10

−12

After irrad.
Before irrad.

Anode

Gate

0

20

40

60

80

Voltage (V)−2Current density (mA cm )Fig. 1. I-V characteristics of FEA in triode configuration before and after -ray irradiation.

EXPERIMENTS: The FEAs were fabricated at National Institute of Advanced Industrial Science and Technology. Photoconducting CdTe/CdS diodes were fabricated at National Institute of Technology, Kisarazu College. The irradiation of -rays to these devices was performed at Kyoto University Research Reactor Institute,
Co-60 Gamma-ray Irradiation Facility. Irradiation of
-ray to the FEAs was performed in a vacuum vessel
made of glass. Current-voltage (I-V) characteristics of the
FEA and CdTe/CdS photodiode were investigated before
and after -ray irradiation. The dose of irradiation was
between 60 and 200 kGy, depending upon the sample
position during the irradiation.

24
20

After irrad.
Before irrad.

16
12
8
4

Substrate type0
0.0 0.1 0.2 0.3 0.4 0.5 0.6
Voltage (V)Fig. 2. I-V characteristics of CdTe/CdS diode in
substrate-type configuration before and after –ray
irradiation.
ACKNOWLEDGMENT: A part of this study is theresult of “Development of radiation tolerant compact
image sensor with a field emitter array”, carried out under the Initiatives for Atomic Energy Basic and Generic
Strategic Research by the Ministry of Education, Culture,
Sports, Science and Technology of Japan.

RESULTS: Fig. 1 shows the I-V characteristics of the
FEA in a triode configuration. No significant change of
the I-V characteristics was observed even after the –ray
irradiation with the dose of 125 kGy. Fig. 2 shows the I-V
characteristics of the CdTe/CdS photodiode prepared on agraphite substrate (Substrate-type configuration). Also forthis case, no significant change of the I-V characteristics
was observed after the –ray irradiation with the dose of
75 kGy. Taking the fact that semiconductor image sensors
have the life of 100 kGy, the FEA and thephotoconducting CdTe/CdS diode have sufficient toler-

REFERENCES:[1] M. Nagao, Proc. of the 21st International Display
Workshops, Dec. 3-5, 2015, Niigata (2015) 588-590.
[2] T. Okamaoto, R. Hayashi, S. Hara, Y. Ogawa, Jpn. J.
Appl. Phys., 52 (2013) 102301/1-3.

採択課題番号 26002
耐放射線性に優れた微小真空冷陰極アレイ撮像素子の開通常採択（京大院・工）後藤康仁、高木郁二、秋吉優史、辻 博司（静岡大・電研）根尾陽一郎（京大・原子炉）佐藤信浩

110CO4-2

Sub-Terahertz Absorption of Ionic Liquid

T. Awano and T. Takahashi1

30Faculty of Engineering, Tohoku Gakuin University
Research Reactor Institute, Kyoto University[1-Ethyl-3-methylimidazolium][BF 4]-1

ABSORPTION COEFFICIENT (cm )

1

295K
273K
258K
227K
-158K

20

for 91K

10

0

4

6
8
10
-1
WAVE NUMBER (cm )12Fig. 1. Absorption increment spectra of [Emim][BF4]. The
baseline is the absorption spectrum at 91K.
-1

ABSORPTION COEFFICIENT (cm )INTRODUCTION:
We have observed millimeterwave absorption bands around 6 and 8 cm-1 in
AgI-superionic conductive glasses. These bands werealso observed in CuI-superionic ones[1-3]. These bands
seems to be due to collective motion of conductive ions,although how conduction ions moves in correlation is notclear.
Ionic liquid (IL) is molten salt at room temperature. It
is interesting to compare ionic motion in ionic liquids
with those in superionic conductor.
Recently, we have measured sub-terahertz absorption
spectra of N,N-Diethyl-N-methyl-N-(2-methoxyethl)
ammonium tetrafluoroborate ([DEME][BF4]) and
N,N-Diethyl-N-methyl-N-(2-methoxyethl)ammoniumbis(trifluoromethanesulfonyl)imide([DEME][TFSI])[4]. Two absorption bands were observed around 6 and 8
cm-1, which are almost coincident with those in
AgI-superionic conductive glasses. These bands havealmost equal peak positions and intensities in both ILs.
This means that these absorption bands are due to cation
motion. However, thermal change of these bands are different. This difference seems to be due to the differenceof their phase transition temperatures and solid states.
The former becomes glassy solid under 182 K. The latterbecomes crystal.
To investigate these difference among ILs, measurements of absorption spectra of several ILs have been executed.

20

10

EXPERIMENTS: Ionic liquids (Tokyo Kasei. co., inc.)were spread into filter paper. Transmission spectra of
single and double papers with ionic liquids were measured at room temperature and low temperatures. Absorption spectra were obtained by subtraction of them.
RESULTS:
Fig. 1 shows absorption spectra of
1-Ethyl-3methylimidazolium
tetrafluoroborate([Emim][BF4]). This ionic liquid becomes solid under
210 K. Fig. 2 shows absorption spectra of
1-Ethyl-3methylimidazoliumbis(trifluoromethanesulfonyl)imide([Emim][TFSI]) .
Temperature dependence was different in these ionic liquids. The intensity of the absorption band of the former
IL decreased gradually at temperatures above 227 K. On
the other hand, that of the latter IL decreased rapidly attemperatures below 213 K. This difference seems to be
due to the difference of their phase transition temperatures and glass or crystal structure of solid states of theseILs due to the anion difference.

0[1-Ethyl-3-methylimidazolium][TFSI]
292K
213K
158K
for 89K

4

6
8
10
-1
WAVE NUMBER (cm )12Fig. 2. Absorption increment spectra of [Emim][TFSI].
The baseline is the absorption spectrum at 89 K. The
spectrum of 158 K was almost coincident with thebaseline.
REFERENCES:[1] T. Awano and T. Takahashi, J. Phys. Conf., 148(2009) 012040/1-4.
[2] T. Awano and T. Takahashi, J. Phys. Soc. Jpn. 79
Suppl. A (2010) 118-121.
[3] T. Awano and T. Takahashi, Proceedings of the 13th
Asian Conference on Solid State Ionics, (2012) 569-576.
[4] T. Awano and T. Takahashi, KURRI Progress Report
2013, CO4-5.

採択課題番号 26015 超イオン導電体におけるコヒーレントミリ波誘起イオン伝導の検証 通常採択
共同通常
（東北学院大・工）淡野照義、（京大・原子炉）高橋俊晴
111

CO4-3Generation of Circular Polarization using Linearly Polarized
Coherent Transition Radiationof the detector.
RESULTS: The observed polarization diagrams of CTRs
from WG1 (horizontal component) and WG2 (verticalcomponent) are shown in Fig.1 and 2, respectively. In
these figures the degrees 0 and 180 represent the verticalplane, and 90 and 270 represent the horizontal plane.
These results demonstrate that CTR from the wire gridhas perfect linear polarizations. The observed
polarization diagram of the superposition of these two
CTRs is shown in Fig.3. This figure represents that thecircular polarized CTR was generated.

T. Takahashi
Research Reactor Institute, Kyoto University
INTRODUCTION: In recent years various types ofcoherent radiation emitted from a short bunch of
relativistic electrons have attracted a considerable
attention as a bright light source in the THz-wave andmillimeter 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 oftransition radiation (TR) emitted from a metallic screen isaxially symmetric with respect to the trajectory of anelectron beam. In my previous reports [1, 2] the propertyof CTR emitted from a pair of wire-grid radiators withthe different polarization was experimentally investigatedin order to develop a new technique of generation of
circular polarized THz radiation. Circularly polarized
light has been useful in the circular dichroism
spectroscopy. Shibata et al. has developed a technique ofgeneration of circularly polarized millimeter-wave
radiation with the phase difference between the forward
TR and the backward one [3]. However, it was difficult tocontrol the polarization degree in that technique. In thisreport circularly polarized CTR has been generated witha new technique. With this technique the polarization
degree is able to be controlled precisely.
EXPERIMENTAL PROCEDURES: The experiment
was performed at the coherent radiation beamline [4] at
the 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, 33
ns, and 20 Hz, respectively. The average current of theelectron beam was 0.5 A. Two wire-grid polarizers(WG1 and WG2) 10 m thick with 25 m spacing wereused in order to generate the CTR with horizontal andvertical components, respectively. Each CTR was
superposed with phase difference through the opticaldelay system. Although a Martin-Puplett-type
interferometer is usually used as a spectrometer, agrating-type monochromator was used in this experiment.
The monochromator was set for the wavelength of 2.3
mm. The CTR was detected by a liquid-helium-cooled Sibolometer. In order to analyze the polarization degree awire-grid polarizer with a rotary holder was used in front

REFERENCES:[1] T. Takahashi, et al., KURRI-PR 2012 CO4-15.
[2] T. Takahashi, et al., KURRI-PR 2013 CO4-12.
[3] Y. Shibata et al., Rev. Sci. Instrum. 72 (2001) 3221.
[4] T. Takahashi et al., Rev. Sci. Instrum. 69 (1998)
3770.

Fig.1. Polarization diagram of CTR from WG1.

Fig.2. Polarization diagram of CTR from WG2.

Fig.2. Polarization diagram of superposed CTR from
WG1 and WG2.

採択課題番号 26016

コヒーレント遷移放射を用いたミリ波領域円偏光制御と近接場分光法に関する研究（京大・原子炉）高橋俊晴、窪田卓見

112

通常採択

CO4-4

Basic Study on Radiation-induced Luminescence from Natural Mineral

H. Fujita, M. Sakamoto1, T. Saito1

1 min at 50 ºC intervals ranging from 150 to 300 ºC as
preheat treatment. Each remnant of the samples was kept
in dark room without preheating treatment. After the ESR
measurements, all luminescence measurements were
performed using a JREC automated TL/OSL-reader system installed with a small X-ray irradiator (Varian,
VF-50J tube). All preparations were carried out under
dim red light.

Nuclear Fuel Cycle Engineering Laboratories, JAEA
1
Research Reactor Institute, Kyoto University
INTRODUCTION: Dielectric materials such as natural minerals emit radiation induced luminescence such as
thermoluminescence (TL) and optically stimulated luminescence (OSL). OSL is a well-established tool formeasuring radiation doses in unfired sediments [1]. It hasfeatures in common with TL which has long been used inmeasuring radiation doses [2]. Both TL and OSL dosimetry with white mineral do not need to be specially installed in advance, prior to dose estimation. Quartz is an
excellent material for use in dosimetry, because of its
almost ubiquitous availability including an accidental
place. Feldspar is an extensive ternary family of minerals
appropriate for OSL and TL dosimetry as they display astrong luminescence and are quite common in the Earth’s
formation. However, the detailed emission mechanisms
of TL and OSL from natural minerals such as natural
quartz and feldspar are not yet clear. In this study, theemission mechanisms of TL and OSL were investigatedin conjunction with various radiation-induced phenomena
after annealing treatments of quartz samples, involving
TL, OSL and electron spin resonance (ESR) measurements.

RESULTS: In this research, the ESR signals of Al
centers and Ti centers ([TiO4/H+]0, [TiO4/Li+]0 and[TiO4/Na+]0) were detected in the annealed quartz samples. Al centers are hole-trapped centers and Ti centers
are electron-trapped centers. Fig. 1 shows the intensitychanges of the Al
centers and the Ti
centers. ESR signal
intensity of Al centers decreased withpreheating temperatures, gradually.
On the other hand,
ESR signal intensity of Ti centers
showeddifferent
tendency from the
ESR intensity of Al
centers. The intensity of Ti centers
increased or was
Fig.1 Tendency of ESR signal intensity
constant up to 150with preheating temperature.
ºC of preheating
temperature. After
heating over 150 ºC, the intensity of Ti center decreased
with preheating temperatures. The results agreed to ourprevious results. However, the intensity tendency of Ti
centers was different between two quartz samples.
TL and OSL signals were measured using all kinds ofquartz samples. However, their data was not evaluated,completely. Therefore, the data analysis will be conducted in 2015.
In this research, the luminescence emission mechanism
could not be identified. Therefore, further work is necessary to identify luminescence mechanism using ESR
measurement and annealing experiment.

EXPERIMENTS: Two surface soil samples to 5 cm
depth were collected at different places in Ibaraki. Natural quartz samples were extracted from the soils by ausual treatment of 6M hydrochloric acid (HCl), 6M sodium hydroxide (NaOH) followed by 60 min of concentrated hydrofluoric acid (HF). The etching treatment with
HF solution was at room temperature. Further purification of the quartz grains was performed by hand selection
for the sake of elimination of feldspar grains as low as
possible. The purified quartz samples were sieved to adjust the grain sizes ranging from 150 m to 250 m in adiameter for ESR spectrometry, TL and OSL measurements. The quartz samples were annealed at 800 ºC for
24 hours in an electric furnace. The annealed quartz samples were irradiated a dose of 1 kGy with 60Co source(0.73 kGy/h at D-30 cm) at room temperature at Kyoto
University Research Reactor Institute (KURRI). The irradiated samples were stored at room temperature for one
day to eliminate afterglow emission in dark room. The
ESR measurement was carried out using an ESR spectrometer (Jeol Ltd., JES-TE 200) at −196 ºC. Prior to the
ESR measurements, the quartz samples were annealed for

採択課題番号 26027

REFERENCES:[1] Huntley, D. J., et al., Nature 313, 105-107 (1985).
[2] Mckeever, S. W. S., Cambridge University Press,
Cambridge, 103-105 (1985).

天然鉱物からの放射線誘起ルミネッセンスの基礎的研究（原子力機構、核サ研）藤田博喜（京大・原子炉）阪本雅昭、齊藤毅

113

通常採択

CO4-5Complex Structure of Ions Coordinated with Hydrophilic Polymer. 15.
Applied Discussion with Ionic Behavior in Hydrophobic Matrixes.
even with aqueous solvents. On the other hand, increasein mass (m, relative mass at each stage to non-doped
sample) was much less than one for the previous hydrophilic matrixes: m less than 2%.
Furthermore, not only deep diffusion of polyiodide in“(1st) iodine doping” but “elution out” of polyiodide orAg+ ion in “(2nd) Ag-doping”.(Fig.1&2, right) Suchbehavior is analogous to “Stage III” which is observed inexcessive “Ag-doping” to iodine-doped hydrophilicpolymers.[6]These results indicate that existence of polyiodide inpolymeric materials can let ionic diffusion overcome
general activation barrier.
ACKNOWLEDGEMENT: SEBS elastomers as hydrophobic samples, AR-770C and AR-830C, were presented
by Aron Kasei Co.Ltd. The authors express great gratitude for them to inspire unexpected viewpoints.

A. Kawaguchi , Y. Morimoto
Research Reactor Institute, Kyoto University
INTRODUCTION: We have reported composite structure brought by in situ preparation through "secondary
doping" by diffusion of metallic ions into iodine-dopedhydrophilic polymers. Polyiodide ions, Inm- (m, n: integer, n ≠ 1 ), which have been as solutes in aqueous solution, can be diffused into the polymers through immersing operation at room temperature. Or, the polymer
matrix previously iodine-doped enhances following diffusion of other molecules or ions into matrix polymer; if
the additional ion makes precipitates of inorganic saltwith iodide, hybrid composite can be achieved without
melting, nor casting, nor synthesizing.[1-3]Such singularity suggests microscopic behavior of polymer chains as “pseudo solvents”, where ionic diffusion in
nano-scale can be achieved or enhanced under affinity
with polymer matrix keeping its structure: chain orientation, crystalline structure, self-organization,,etc. However, even if matrix is composed by “hydrophilic” polymers, their polarization or ionic affinity are not matchedfor ordinary hydrophilic solvents, such as water, ethanol,,etc.; hydrophilicity of polymeric matrixes should bemuch lower than that of hydrophilic low molecules, andthat is a reason for general difficulty for charged ions todiffuse into the matrixes.
If so, observed rapid diffusion of polyiodides (“(1st) iodine doping”) or additional diffusion of metallic ions(“2nd doping”) should consistent with hydrophobicity ofmatrixes not only their hydrophilicity.[4,5] Then, similar procedures for “(1st) iodine doping” or “(2nd) Ag+ ion
doping” in hydrophobic matrixes were investigated ascomparison with the previous results in hydrophilic matrixes.
EXPERIMENTS: Commercial "SEBS"-elastomer,
AR-770C and AR-830C (Aron Kasei) were used as hydrophobic matrixes, which are composed of both polystyrene (hard segment) and polyethylene-polybutylene
co-polymer (soft segment).
Iodine doping was achieved with I2-KI(aq)/3.0N (for 22
hrs., at R.T.) and secondary doping was done with AgNO3(aq)/0.25M (for 30min., at R.T.).
RESULTS: Present matrixes are just "hydrophobic" depending on their chemical components; generally, theiractivity to aqueous solution is so low that ionic diffusion
or interaction should be negligible. However, ionic diffusion from aqueous solution into the hydrophobic matrixes was explicitly observed in coexistence of polyiodide ions. As shown in Fig. 1 and 2, “(1st) iodine
doping” and “(2nd) Ag-doping” easily advanced into bothhydrophobic matrixes in time of less than an hour at R.T.

Fig. 1. AR-770C iodine-doped with I2-KI(aq) (left)
and following “(2nd) Ag-doping” with AgNO3(aq)(right).

Fig. 2. AR-830C iodine-doped with I2-KI(aq) (left)
and following “(2nd) Ag-doping” with AgNO3(aq)(right).
REFERENCES:[1] A. Kawaguchi, Sens. Actuators B, 73 (2001) 174-178.
[2] Y. Gotoh, et.al., Polym. Prep. Jpn., 51 (2002),
2259-2259.
[3] patent. JPN-5444559 (2014).
[4] KAWAGUCHI Akio, et.al., SPring-8 User Exp. Rep.
5 (2000A), 354-354. (2000)[5] A. Kawaguchi, et.al., Macromol. Sym., 202, 77-83.
(2003)[6] A. Kawaguchi, Polym. Prep. Jpn., 62, 5116-5117.

(2013)

採択課題番号 26052 親水性高分子－金属塩ナノコンポジットの調製と構造（京大・原子炉）川口昭夫、森本幸生

114

一般通常
通常採択

CO4-6

Elucidation of Tritium Dynamics in Neutron Irradiated Tungsten

Y. Oya, M. Sato1, K. Yuyama1, T. Miyazawa2, R. Okumura3, Y. Iinuma3, T. Fujii3 and H. Yamana3

and voids [1-3]. No large difference for Peak 1 was foundamong 0.01 and 0.1 dpa Fe2+ irradiated samples, indicating that the retention of D adsorbed on the sample surface
or trapped by dislocation loops would be almost saturated.
However, for 0.1 dpa sample, major D desorption stage
was shifted toward higher temperature side at 850 K,
showing that voids would be more stable D trapping sites.
In the case of fission neutron irradiation, only D retention
as Peak 1 was increased, but its retention was almost thesame as Fe2+ irradiated W, indicating that the dislocation
loops for D trapping would be almost the saturation andno vacancy for D trapping was produced into the sample
due to its lower damage concentration, or rhenium (Re)which produced by the transmutation caused by thethermal neutron irradiation, would contribute on the enhancement of D re-emission, although vacancies were
produced. According to Ref. [4], due to the smaller sizeof Re atom than that of W atom, substitutional Re atom
tends to bound to self-interstitial atoms (SIA) because
their lattice strain field is opposite. Once the Re-SIA
complex is formed, the mobility of the SIA decreases,
leading to the enhancement of vacancy-interstitial recombination.

College of Science, Academic Institute, Shizuoka University
1
Graduate School of Science, Shizuoka University
2
Faculty of Science, Shizuoka University
3
Research Reactor Institute, Kyoto University
INTRODUCTION: Tungsten (W) is a candidate material for the plasma facing components in the fusion future reactors due to the lower hydrogen isotopes retention.
In a fusion reactor, W will be exposed to 14 MeV neutrons produced by the D-T fusion reaction during theplasma operation. Irradiation defects will be introducedby neutrons where hydrogen isotopes would be stably
trapped, leading to the enhancement of fuel retention.
Therefore, it is important to evaluate the hydrogen isotopes retention in neutron irradiated W. In this study, thedeuterium retention behavior in neutron irradiated W wascompared with that in heavy ion implanted W which has
typical defects such as dislocation loops, vacancies andvoids.

Desorption rate / 1017 D2 m-2 s-1

1.5

EXPERIMENTS: Disk type W (6 mmφ×0.5 mmt) purchased from A.L.M.T. Corp. Ltd was used as the sample.
The samples were heat-treated at 1173 K under ultrahighvacuum to remove the impurity and damages introducedby the polishing process. The neutron irradiation for the
sample was performed at Pn-2 port in Kyoto University
Research Reactor Institute (KUR) with the damage up to
4.3 × 10-4 dpa (displacement per atom). For the heavy ion
irradiation, 6 MeV Fe2+ was irradiated into the samples atroom temperature with the damage concentrations of 0.01
and 0.1 dpa by Takasaki Ion Accelerators for Advanced
Radiation Application (TIARA) at Japan Atomic Energy
Agency (JAEA). Thereafter, the samples were transferred to Shizuoka University for D2+ implantation. The
samples were irradiated at R.T. with 1 keV D2+ with aflux of 8.75×1017 D m-2 s-1 to a fluence of 1.0×1022 D m-2.
The D desorption behavior was evaluated by thermal
desorption spectroscopy (TDS) from room temperature
up to 1173 K and 1273 K for Fe2+ irradiated samples andneutron-irradiated sample, respectively, with the heating
rate of 0.5 K s-1.

1.0

Peak 1 Peak 2 Peak 3

Peak 4

un-damaged
Fe2+0.1dpa
0.01 dpa
fission neutron

0.5

0.0

400

600
800
Temperature / K

1000

Fig. 1. D2 TDS spectra for various damaged W.

REFERENCES:[1] Eleveld H and Van Veen A J. Nucl. Mater. 191(1992) 433-438.
[2] Iwakiri H et al., J. Nucl Mater. 307-311 (2002)
135-138.
[3] Luo G N et al., Fusion Eng. Des. 81 (2006) 957-962.
[4] Hasegawa A et al., Fusion Eng. Des. 89 (2014)
1568-1572.

RESULTS: D2 TDS spectra for various damaged W wereshown in Fig. 1. The D desorption peaks consisted offour peaks at 400 K, 550 K, 650 K, 850 K corresponded
to the adsorbed on the sample surface or trapped by dislocation loops, trapped by vacancies, vacancy clusters

採択課題番号 26063 中性子照射タングステンにおけるトリチウムダイナミックスの解明 通常採択
（静大院・理）大矢恭久、佐藤美咲、湯山健太（静大・技術）宮澤俊義（京大・原子炉）奥村良、
飯沼勇人、藤井俊行、山名元115

CO5-1

Central Diameters and Concentrations of Element in the
Atmospheric Aerosols at Sakai,Osaka.

From relations between the d50 and elemental
concentrations we have found that Zn, V, Br, Mo,Sb,As
Radiation Research Center, Osaka Prefecture University, have fine d50 (<=2.5μm) those are Zn(0.9～1.8μm),
1Research Reactor Institute, Kyoto University
V(0.28～0.48μm), Br(0.34～0.59μm), Mo(0.24～1.1μm),
Sb(0.957～0.94μm), As(0.53～1.5μm).
Central diameters and concentrations of
Al,Na,Fe,Ca,Ti,Ba,Cr,Ce,Co,Th,Hf,Eu have coarse
elements(Na,Al,Cl,K,Ca,Ti,V,Cr,Mn,Fe,Co,Ni,Zn,As,Br, d50(>=2.5μm) those are Al(4.6～6.0μm), Na(3.7～4.3μm),
Fe(3.5～5.1μm), Ca(4.7～6.2μm), Ti(4.0～5.9μm), Ba(2.2
Rb,Mo,Sb,Cs,Ba,La,Ce,Sm,Eu,Hf,W and Th) in the～4.1μm), Cr(2.6～4.9μm), Ce(3.0～4.7μm),Co(2.4～
atmospheric aerosols collected at Sakai, Osaka in 2012
have been obtained. We have collected aerosols separated 4.6μm), Th(4.0～6.2μm), Hf(4.5～5.4μm),Eu(4.4～by the 9 diameter ranges(<0.43,0.43～0.65,0.65～1.1,1.1～ 5.6μm),. Cl,K,Mo,Ni,W, La,Cs have coarse and fine d50
2.1,2.1～3.3,3.3～4.7,4.7～7.0,7.0～11,>11μm) using
depending on the sampling period. The variation causechanges of the main constituents in fine d50 depending onAndersen sampler on one week periods (P1:Feb.14-21,
P2:Apr.03-10, P3:Jun05-12, P4:Aug.07-14, P5:Oct.09-16, the sampling period like that, K, Zn,Mn on P1 , Zn on P2 ,P6Dec.11-18: in 2012).To collect the samples completely K ,Zn on P3, Zn on P4, K, Zn on P5, Cl,K,Zn on P6 .
and reduce an affect of contamination we have put
In the fine d50 elements ordered by high to lowpolyethylene sheet(80mmΦ, ～1mg/cm2) on the each stage concentration are Cl,K,Zn,Mn,V,Br,Ni,Mo,Sb,As, W, La ofof the sampler.
which order changes on the sampling period.
The element concentrations were analyzed by neutron
activation analysis using Kyoto University Nuclear Reactor
on following irradiation conditions ( In Pn1 120sec for
Al,Cl,Ca,V,Mn, In Pn2 30min for Co, Ni, Zn, As,Br, Rb,
Mo,Sb,Cs,Ba,La,Ce,Sm,Eu,Hf,W,Th).Gamma ray
spectrum from each irradiated samples were measured by
Ge-Solid state detector and 4096channel multiple pulse
height analyzer. The measuring time(2000～20000sec) andstarts of measurements are determined by the gamma rayintensity of each sample.
From the concentration results in each particle diameter
range we have determined the central diameter(d50) which
is a diameter of 50% accumulation concentration summingby the each particle diameter range concentration(Fig.1).
From the concentrations in each diameter range we get ascatter graph of d50 and total concentrations of eachelement on 6 sampling periods(Fig.2).
N.Ito, A.Mizohata , R Okumura1 and Y Iimura
Iinuma11

Fig.2 Scatter graph of d50 and total
concentrations for each elements in theaerosols collected 2012 at Sakai.

Fig.1 Example of accumulation curve and central
diameter(d50) on concentrations of K(Feb14-21 2012)by aerosol diameter in 9 size ranges.

採択課題番号 26011
大気エアロゾル粒子のキャラクタリゼーション( 大阪府大地域連携 ) 伊藤憲男、溝畑 朗 ( 京大原子炉 ) 奥村良、飯村勇人
奥村良、飯沼勇人
116

通常採択
共同通常

CO5-2

Study of Earth and Planetary Matters by Thermoluminescence
The induced TL of unequilibrated ordinary chondrites
has been usually measured above room temperature.
Then this time low temperature TL (-150~ 0 oC) were
investigated to distinguish TL properties between primitive chondrites and secondary altered chondrites. TL
glow curves of a primitive ordinary chondrite ofA881244 (L3.0) and remarkable shocked chondrite ofA8811255 is shown in Fig.1. TL glow curves of a primitive ordinary chondrite of A881357 (L or LL 3.3-3.4) anda moderate shocked chondrite of A880708. There are two
peaks near -120 and -80oC lower than room temperature.
However we could not find clear difference in TL propertied between primitive chondrites and secondary alteredchondrites.

K. Ninagawa, H. Nishido and S. Hamada
Okayama University of Science
LOW TEMPERATURE TL OF ORDINARY
CHONDRITES: Induced TL (thermoluminescence), theresponse of a luminescent phosphor to a laboratory doseof radiation, reflects the mineralogy and structure of thephosphor, and provides valuable information on themetamorphic and thermal history of meteorites. Thermal
metamorphism causes the production of feldspar, themajor TL phosphor in ordinary chondrites, by the devitrification of feldspathic mesostasis. Primitive chondrites of
petrologic subtype ≦ 3.4 with coefficient of variations( as a percentage of the mean) over 50%, of fayalite in
the olivine have low TL sensitivities under 0.1. The sensitivity of the induced TL is usually used to determine
petrologic subtype of unequilibrated ordinary chondrites[1]. On the other hand, TL sensitivity decreases 10-foldafter shock-loading to 25-32 GPa [2], and terrestrial
weathering makes TL sensitivity decrease 16-fold at
maximum in Antarctic chondrites [3]. Then some secondary altered chondrites were reported to have low TL
sensitivities, equivalent to primitive chondrites [4].

LOW TEMPERATURE TL OF UREILITE: The
ureilites are a major group of primitive achondrites. They
are high fractionated rocks from an achondrite parent
body. Ureirites are olivine-pyroxene rocks with interstitial C (graphite and microdiamonds) mixed with metal,
sulfides, and minor silicate. Most ureilites are essentiallydevoid of feldspar [6]. This time we measured induced
TL of five ureilites to check TL properties of ureilites.
Fig.3 shows TL glow curve of Dar al Gani 319 andNWA3223. There were two large peaks at -100 and 0oC.
Ureilite

A881244 (L3.0)
A881125 remarkable shocked

700

12000
TL Intensity (cps)

TL Intensity (cps)

600
500
400
300
200

-100

-50

0

50

100

150

200

250

300

6000
4000

A880708 moderate shocked

3500
3000
2500
2000
1500
1000
500
0

50

100

150

200

250

300

350

Temperature (oC)Fig.2. TL glow curves of A881357 and moderate shockedchondrite of A880708. The different peaks at 50 and 150
o
C reflected to disordering of feldspar.

採択課題番号 26024

0

50

100

150

200

250

300

350

REFERENCES:[1] Sears et al., Proceedings of Lunar and Planetary Science 21 (1991) 493-512.
[2] Hartmetz et al., Proc. 17th Lunar Planet. Sci. Conf. (J.
Geophysical Research), 91, (1986) E263-E274.
[3] Benoit and Sears, J. Geophys. Res., 104, (1999)
14159-14168.
[4] K. Ninagawa et al., Antarctic Meteorite Research, 15(2002) 114-121.
[5] K. Ninagawa et al., Antarctic Meteorite Research 18(2005) 1-16.
[6] Weisberg et al. Meteorites and the early solar System
II, The University of Arizona Press, (2006) 19-52.

A881357 (L or LL3.3-3.4)

-50

-50

Fig.3. TL glow curve of ureilites, Dar al Gani 319 andNWA3223.

4000

-100

-100

Temperature (oC)Fig.1. TL glow curves of a primitive ordinary chondriteof A881244 (L3.0) and remarkable shocked chondrite ofA8811255.

TL Intensity (cps)

8000

0
-150

350

Temperature (oC)0-150

NWA 3223

10000

2000

100
0
-150

Dar al Gani 319

14000

800

熱ルミネッセンスによる地球惑星物質の研究（岡山理大）蜷川清隆，西戸裕嗣，濱田聖矢

117

通常採択

CO5-3

Evaluation of Redox Conditions at Dredged Trenches in Tokyo Bay
by the Concentrations of Elements in the Sediments

T. Yamagata, K. Shozugawa, R. Okumura1, K. Takamiya1
and M. Matsuo

trations of Fe and Mn in sediments were almost constantfrom the surface to the lower layers. It is well-known factthat the concentrations of Fe and Mn in sediments decrease due to eluviations of Fe2+ and Mn2+ when condition of seawater is reductive like hypoxia. The results
indicate that the redox conditions of the surface of sediments were not so reductive as those in August 2011 [4].
On the other hand, we calculated Th/U and Ce/U ratios
likewise Honda et al [5], and the depth profiles of theratios in sediment are shown in Figure. The Th/U andCe/U ratios in the upper layers (7-8 cm from the surface)were comparatively high, and the ratios settled down toalmost constant lower values below 8 cm in depth at mostsites. It is known that the concentrations of Th and Ce in
sediments increase when condition of seawater is oxidative, and the concentration of U increases when conditionof seawater is reductive. It is considered that the sedimentary environment of the upper layers is more oxidative than that of the lower layers. And focusing on theredox potential around U(VI)/U(IV), the method using
Th/U and Ce/U ratios is well reflecting the redox states,
because those of U, Th, Ce are thought to be preserved
from the time of sedimentation.
As mentioned above, the method measuring the concentrations of various elements by INAA and focusing on
different redox potentials of the elements is very useful toevaluate the sedimentary environment related to redox
conditions.

Graduate School of Arts and Sciences, The Univ. of Tokyo
1
Research Reactor Institute, Kyoto University
INTRODUCTION: Hypoxia is water mass with little dissolved oxygen (DO) [1]. In Tokyo Bay there aremany large and deep dredged trenches, especially off thecoast of Makuhari, Chiba. In dredged trenches severe
hypoxia has been observed in summer, but the influenceof dredged trenches on hypoxia is not revealed yet.
Therefore, it is important to estimate the positional andseasonal variations of hypoxia by analyzing sediments.
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]. We haveapplied the elements to evaluate the sedimentary environment in dredged trenches, which are under specificcondition. In this study, sediment cores were collectedfrom the Makuhari dredged trenches and concentrationsof Fe, Mn, U, Th, and Ce in sediments were analyzed byinstrumental neutron activation analysis (INAA).
EXPERIMENTS: The sediment samples were collected at a dredged trench (water depth 17.2 m) and reference site (non-dredged seabed, water depth 9.5 m) off
the coast of Makuhari in Tokyo Bay in August 2013.
Sediments were collected by a core sampler and water
quality data were also obtained.
All cores were cut in the vertical direction at 0.6-3.0
cm intervals in the laboratory, and the samples were desalted and freeze-dried within a week.
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 or 4 minutes at 5 MW,
and then gamma-ray was measured for 1200 seconds by
Ge detector after 3-5 days cooling. Regarding Th and Ce,
samples were irradiated for 20 minutes at 1 MW or 4
minutes at 5 MW, and the measuring time of gamma-ray
was for 9000 seconds after 2-4 weeks cooling.
RESULTS: At the dredged trench surface water (< 9m water depth) had DO about 6 mg/L, and bottom water(> 12 m water depth) had no DO. At both sites, concen-

Figure. Depth profiles of Th/U (left) and Ce/U
(right) ratios in the sediments collected from Tokyo
Bay in August 2013.
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 et al., Geochim. Cosmochim. Acta, 45(1981), 855-881.
[4] T. Yamagata et al., J. Radioanal. Nucl. Chem., 303(2015), 1179.
[5] T. Honda et al., Bull. Soc. Sea Water Sci., Japan, 57(2003), 166-180 (in Japanese).

採択課題番号 26028
汽水域および沿岸域堆積物の放射化分析
通常採択（東大・大学院総合）松尾基之、小豆川勝見、山形武広、堀まゆみ、青木隆太朗、渡邊利奈、徐放、
山本駿（京大・原子炉）高宮幸一、奥村良118

CO5-4Characteristics of Synthetic Calcite Thermoluminescence Studied for
Paleoenvironmental Reconstruction of East Asia

N. Hasebe, K. Ito, K., K. Miura1 and M. Ogata1

tration to emit luminescence. The TLCI with small
amount of Fe show colored pixels. However, these pixels may be noises because they are found in all colorzones. Mg added samples emitted no luminescence.
Therefore, Mg would not play significant role in luminescence characteristics.

Institute of Nature and Environmental Technology, Kanazawa University
1
Graduate School of Natural Science and Technology,
Kanazawa University
INTRODUCTION: Luminescence dating observes thenatural accumulated radiation damage caused by radioisotopes such as U and Th as the form of glow after stimulation by heating or lightening. Thermally stimulated
luminescence from calcite shows strong red emission [1].
However, thermoluminescence dating of calcite is lesspopular because of some unknown problems; e.g., sensitivity change of calcite occurred through repeated heatingof samples, possible anomalous fading, difference incharacteristics of luminescence response against different
kinds of radiation (e.g., gamma-ray, beta-ray, alpha-ray,and X-ray). When thermoluminescence characteristics
of calcites are examined using natural occurring calcite,
their response to the various radiations depends on minor
chemistry (Fe, Mg, Mn and Sr). In this study, calciteswith controlled impurity concentrations were synthesized and analyzed to evaluate relationship between multiple impurity concentration and thermoluminescence properties quantitatively.

Fig. 1. The amount of elements measured by
LA-ICP-MS is proportional to the amount of added
elements

EXPERIMENTS: Calcite were synthesized from sodium carbonate (>99.8wt%) and calcium chloride (>95wt%). Iron (II) chloride (>99.0-102.0 wt%), magnesium
chloride (>98.0wt%), and manganese chloride (>99.0wt%) were added at different levels to produce calciteswith different amount of impurity. Chemical compositionof resultant calcite were measured by LA-ICP-MS.
Gamma irradiation was carried out at the 60Co gamma
irradiation facility at Kyoto University Research Reactor.
Then luminescence images were captured by the digital
camera (Inagaki et al., 2010) and luminesce color andintensity were analyzed (Ogata et al., 2014).

$                    
#!"

RESULTS: Except for added elements, all of synthetic
calcite contain ~30 ppm of strontium and ~6 ppm of barium. These elements must be contained in original reagent calcium chloride. Mn-added calcites include molybdenum which amount is proportional to the amount ofadded Mn. Mo must be contaminated to the reagent
manganese chloride. As shown in Fig. 1, measured
amount of impurity is proportional to the amount ofadded impurity.
When thermoluminescence color image (TLCI) was captured, Mn added samples emitted strong red luminescence (Table 1). A sample with high impurity emit noluminescence. There may be some criteria in Mn concen-

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


 
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 
 

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




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


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




"  


 
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

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Table 1. The results of TLCI investigation. Number of pixels in each color zone is counted. R stands
for red, Y for yellow, G for green, B for blue, andgap for other color.
REFERENCES:[1] A. Inagaki et al., J. Geol Soc. Japan 116 (2010)
XIX-XX[2] M. Ogata, Sci. Rep. Kanazawa Univ. 58 (2014) 1-12

採択課題番号 26029	
  東アジアにおける古環境推定のための放射年代測定	 （金沢大・環日本海域セ）長谷部徳子、伊藤健太郎、(金沢大院・自然)三浦知督、小形学	
 
	
 

119

通常採択	
 

CO5-5 Fission Track Ages of Sedimentary Rocks from Accretionary Belt in the Kii Peninsula
H. Ohira and A. Takasu

with that the “Yanase Fault” is important thrust system
which dividing complexes of this area and the Hanazono
complex was exposed to relatively higher temperature
due to deep burial. Almost FT grain ages from the Yukawa complex show entirely older than the estimated depositional period, indicating that sample was not affectedby heating up to enough temperature to reset FT ages. On
the contrary, the youngest age component in the Ryujin
complex (59Ma) is significantly younger than the limit ofdepositional period (68-78Ma). This result probably indicates that most of FT grain ages of Ryujin complex
were reset by thermal affect during burial process to a
deeper level, or the depositional age of the Ryujin complex is actually younger than previous interpretation.
Detail track length measurement will be required for thesolution of above discussion.

Department of Geoscience, Shimane University
INTRODUCTION: Fission track dating was applied for
sedimentary rocks of Kii peninsula, Wakayama prefecture. The aim of this study is to estimate depositional
periods and thermal histories of sedimentary rocks inrelation with burial-uplift processes during accretion
process. In recent study, the Cretaceous Shimanto Belt inthis area is newly divided into several accretionary complexes showing zonal structure, Ryujin, Miyama, Yukawa and Hanazono complexes, from the south to north[1]. FT age variations across the Shimanto belt in the Kii
region and relationship between FT ages and thermal andburial/uplift history has been precisely discussed mainly
for areas of the north side including a part of Hanazono
complex [2].
EXPERIMENTS: Samples collected from each units of
the Shimanto belt were crashed and sieved and heavy
minerals were concentrated by common method. Zircon
and apatite were abundant in almost samples but lessamounts in the Miyama complex. Zircons were mounted
in PFA Teflon, and then polished to reveal entire internalsurface. Samples were etched in a NaOH-KOH eutectic
melt at 225˚C [3] for 20-32 hours and were irradiated atpneumatic tube of graphite facility (Tc-pn) of Kyoto
University Reactor (KUR). FT densities were measured
using optical microscope at 1000× magnification with adry objective 100×．FT ages were calculated by trackkey
program [4].
RESULTS: Fission track grain ages show wide variations in each sample but the youngest modes in histograms show a systematical tendency from south to north,probably corresponding to depositional period and thermal histories during burial-uplift process of each geological unit. Ranges and modes in histograms for each complexes are as follows; Ryujin (53-92Ma; 60Ma), Miyama(57-197Ma; 68Ma), Yukawa (94-300Ma; 126Ma), andHanazono (55-93; 68Ma). FT ages become old fromsouthernmost Ryujin complex toward the northern Yukawa complex, but the Hanazono complex in northernmost district show young age again. The gap of age between the Yukawa and Hanazono complex and rejuvenation of FT age in the Hanazono complex is compatible

Fig.1 FT age histogram and geological map with each complex
boundary [5].

[1] Suzuki H. and Nakaya S., 2012, The Assoc. Geological Collaboration in Japan, Monograph 59, 273-282(in Japanese with English abstract).
[2] Hasebe N. and Tagami T., 2001, Tectonophysics 331,247-267.
[3] Gleadow A.J.W. et al., 1976, Earth and Planetary
Science Letter, 33, 273-276.
[4] Dunkle, I., 2002, Computer & Geosciences, 28, 3-12.
[5] Suzuki H., 2012, The Assoc. Geological Collaboration in Japan, Monograph 59, 101-110 (in Japanesewith English abstract)

採択課題番号 26036 フィッション・トラック年代測定法による岩石の熱履歴解明に関する研究 通常採択
（島根大・総合理工）大平寛人，高須 晃
120CO5-6 Trace Amounts of Halogens (Cl, Br and I) in Manganese Nodule Reference Materials
M. Ebihara and S. Sekimoto1

Our RNAA data for Nod-P-1 and Nod-A-1 are not consistent with the literature data obtained by ICP-SFMS for
both bromine and iodine. As for iodine the ICP-SFMS
values are lower than the RNAA values. Such an inconsistency between RNAA values and ICP-SFMS values
also may be derived from the loss of iodine in the aciddigestion procedure with heating by the microwave. To
prevent the loss of iodine, the digestion solution should
not be heated in principle, or heating of the digestion solution must be achieved with extreme care. Regarding
bromine, on the other hand, the ICP-SFMS values arehigher than the RNAA values by a factor of about three tofive. Such an inconsistency between RNAA values and
ICP-SFMS values may be due to the ability of thisICP-SFMS instrument, especially to background [4].
Bromine is determined by ICP-SFMS and/or ICPMS
using the isotope 79Br and 81Br. The mass of those twobromine isotopes is next and very close to the biatomic(40Ar40Ar)+ molecule of mass 80. Since argon is so abundant in the plasma of the ICP-SFMS and/or ICPMS, thecombination of two 40Ar ions causes a large peak at mass
80 whose peak tail could interfere with either stable isotope of bromine. Additionally, there are several potential
interferences on 79Br and 81Br; (40Ar39K)+, (63Cu16O)+ and(40Ar38Ar1H)+ interference with 79Br and (40Ar41K)+,(65Cu16O)+ interference with 81Br signals, respectively [4].
To quantify 79Br successfully without interference of(40Ar39K)+ and (63Cu16O)+ nor of (40Ar38Ar1H)+, the
ICP-SFMS instrument should be operated in resolution(m/m) of >10000 or >5000, respectively. (A required
resolution for successful quantification of 79Br is explained in the Supporting Information.) In case of theliterature values for bromine, however, the ICP-SFMS
instrument was operated in medium resolution mode(m/m=4500) for 79Br, and interference of (40Ar39K)+ and(63Cu16O)+ cannot be removed from 79Br signal. A possible explanation of higher bromine values in ICP-SFMS
than in RNAA could be an overestimation due to the interference at mass 79 in the ICP-SFMS instrument. Since
the ICP-SFMS operation in high resolution mode (HRM)
is generally the operation in resolution (m/m) of
9000-10000, it is fundamentally impossible to quantify
79
Br successfully without interference of (40Ar39K)+ and63( Cu16O)+ even using the HRM. This suggests that bromine-separation as a pretreatment of samples is essential
for bromine-determination using ICP-SFMS and/or
ICPMS.

Graduate School of Science, Tokyo Metropolitan University
1
Research Reactor Institute, Kyoto University
INTRODUCTION: Accurate and reliable data of halogen abundance have been rarely reported for terrestrial
samples, such as manganese nodule materials. Since halogens differ in volatility from element to element, theircontent and relative abundance are highly informative
when discussing the petrogenesis of such samples. Recently, we have improved the radiochemical neutron activation analysis (RNAA) procedure for trace amounts of
halogens (Cl, Br and I) [1]. In this study, our RNAA wasapplied to two manganese nodule materials that areavailable in U.S. Geological Survey (USGS) and then,our RNAA values were compared with the literature values.
EXPERIMENTS: Trace amounts of Cl, Br and I in thetwo manganese nodules (Nod-P-1 and Nod-A-1) were
determined by RNAA. The RNAA procedure is described
elsewhere [1-2]. Those samples were repeatedly analyzed
more than two times.
RESULTS: The two manganese nodules (Nod-P-1 andNod-A-1) analyzed using RNAA in this study were also
analyzed using inductively coupled plasma double focusing sector field mass spectrometry (ICP-SFMS) [3]for bromine and iodine. Our RNAA values and the
ICP-SFMS values are shown in Table 1. Before analysis
by ICP-SFMS, the nodule materials were subjected to theacid digestion procedure, in which the nodule materials
are heated with the mixture of concentrated nitric, hydrochloric and hydrofluoric acids by using microwave.
The digestion solution was diluted appropriately and thenintroduced into the ICP-SFMS instrument.
Table 1: Cl, Br and I contents in USGS manganese nodule materials analyzed by RNAA in this studya and fromthe LiteraturesampleNod-P-1

Nod-A-1a

RNAA(n = 4)
ICPSFMS15RNAA(n = 2)ICPSFMS15

Cl(mg kg-1)
1380 ± 140

Br(mg kg-1)
5.93 ± 0.76

I(mg kg-1)
157 ± 17-b30.3 ± 2.2

31.4 ± 0.3

4410 ± 160

14.8 ± 0.5

367 ± 9b40.9 ± 0.7

47.7 ± 3.2-

REFERENCES:[1] S. Sekimoto and M. Ebihara, Anal. Chem., 85 (2013)
63366341.
[2] S. Sekimoto and M. Ebihara, in preparation.
[3] M.D. Axelsson et al., Analyst, 127 (2002) 76-82.
[4] J. Hammerli et al., Chem. Geol., 337-338 (2013)75-87.

Mean values followed by standard deviations (1) (n=3,4). Mean values followed by an uncertainty which issimply the value calculated from two individual uncertainty values. (n=2) bNot reported.

採択課題番号 26043

宇宙・地球化学試料中の微量ハロゲン(Cl, Br. I)の中性子放射化分析（首都大学東京・大学院・理工）海老原 充、白井直樹（京大・原子炉）関本 俊
121

通常採択

CO5-7

Application of Neutron Activation Analysis to Micro Gram Scale of Solid Samples

S. Sekimoto, N. Shirai1, M. Ebihara1

using Allende and JB-1 as reference samples. Hereafter,these experimental runs named run-2 [1] and run-3 [2]are discussed in comparison with the present study, whichis named run-1. It is meaningful to compare the activityof radioactive nuclides used in INAA for two different
reference samples. We discuss the gamma rays counting
rate per unit mass for each target element, hereafter
gamma-ray intensity, among three runs. The gamma rays
counting rate is gamma ray counts per second and correspond to gamma ray energies designated for individual
nuclides (24Na, 46Sc, 59Fe, 140La, 153Sm, 58Co, 60Co, 65Zn
and 51Cr). Those nine nuclides were determined both forAllende and JB-1. Relative gamma-ray intensities of 24Na,
46
Sc and 59Fe in both reference samples are highly consistent for the three runs. Such a consistency can also beseen for Fe reagents. Kong and Ebihara [3] evaluated theconsistency in elemental contents in the mg size of JB-1
and confirmed that JB-1 is well homogenized for its use
in mg. We confirm that Allende can also be used as areference sample for mg scale of sample at least for Na,
Sc and Fe. On the other hand, Allende and JB-1 show asmall inconsistency, most of which may be due to poor
counting statistics for either sample. For example, Allende tends to have relatively low contents of rare earth elements (La and Sm), whereas JB-1 has a low content of
Ni and Zn. Depending upon elemental contents, either
Allende or JB-1 may be used for a reference sample.
There appears an apparent inconsistency in Cr data between the two reference samples, with JB-1 having systematically higher gamma-ray intensity. This isundoubtfully due to an erroneous reference value (425
mg kg-1) of Cr for JB-1. If a proposed value (475 mg
kg-1) [3] is instead used, an excellent consistency can beseen as shown in Fig. 1 for 51Cr.

Research Reactor Institute, Kyoto University
1
Graduate School of Science, Tokyo Metropolitan University
INTRODUCTION: Since instrumental neutron activation analysis (INAA) is a non-destructive and multi-elemental analysis method, it is suitable for precious
samples and, especially, for such specimens as thosehighly desired to be neither physically decomposed nor
chemically dissolved. Meteorites are the best example forsuch samples. Chondritic meteorites (chondrites) and ironmeteorites contain relatively high contents of Co and Ir
compared with those in the earth crust. As Co and Ir havehigh sensitivity in NAA, they can be good markers forthe identification of such extraterrestrial materials. In
NAA of chondrites, a few tens mg of specimen is commonly used. For such a case, a few hundred μg kg -1 of Ir
and a few hundred mg kg-1 of Co can be reliably determined. When an extremely small size (e.g., micro gram)of samples such as micrometeorites recovered on the
Earth surface and tiny particles returned from extraterrestrial asteroids are to be analyzed by INAA, the conventional INAA procedure used for a few tens mg is notsuitable. For such tiny samples, neutron irradiation withhigh neutron flux and long irradiation time (namely, highneutron dose) is required. For the irradiation with highneutron dose, polyethylene bags for holding samples are
not usable because they are prone to radiation damage.
Polyethylene bags are also not suitable for holding tiny
grain samples. It is, therefore, very important to design anappropriate sample holder for irradiating small grain
samples. As we use a relative method for quantification,in this report, the preparation of reference samples andthe evaluation for their suitability are described in detail.

Gamma-ray intensity[108] 40

EXPERIMENTS: Two reference samples with different elemental compositions were used; the Allende meteorite powder (1.66 mg) prepared by the Smithsonian Institution (USMN 3529; split 22 and position 6) and thebasaltic rock reference sample JB-1 prepared by Geological Survey of Japan (1.12 mg). Each sample was sealed
into a synthesized quartz tube (1 mm inner  and 2.7 mm
outer  x 35 mm length), which was then wrapped with
Al foil for the safety. The neutron irradiation was performed for 45 hours at the hydro-irradiation port of Kyoto University Reactor (KUR) in Kyoto University Research Reactor Institute (KURRI) under 1MW operation.

20

AllendeJB-1
JB-1[3]

51

Cr

10

Run-1
Run-2
Run-3
Fig. 1. Gamma-ray intensities of 51Cr in referencemonitors for run-1, run-2 and run-3.
REFERENCES:[1] M. Ebihara et al., Meteorit. Planet. Sci., 50 (2015)
243-254.
[2] M. Ebihara et al., Science, 333 (2011) 1119-1121.
[3] P. Kong and M. Ebihara, Geochem. J., 31 (1997)
339-344.

RESULTS: For quantification in INAA, two reference
samples (the Allende meteorite and the JB-1 basalt) having different elemental contents were used. We haveconducted similar INAA experiments where tiny grain
samples collected by the spacecraft were analyzed by

採択課題番号 26048 京大炉(KUR)における微小隕石及び標準岩石試料の中性子放射化分析 通常採択
（京大・原子炉）関本俊（首都大院理工）海老原充、白井直樹(九大院理)岡崎隆司
122CO5-8Probability distribution of SEL occurred on on-board computer (OBC)
mounted on small-scale satellite
from the ground test is 2.8x105 to 1.4x106 times the
cross-section derived from the on-orbit data.

H. Masui, T. Tomioka, K. Taniwak, M. Cho and K.
Takamiya1
Kyushu Institute of Technology
Research Reactor Institute, Kyoto University

1

INTRODUCTION: Recently universities and venturebusinesses actively develop small-scale satellites. For thesmall-scale satellites, many COTS (Commercial-off-the-shelf) components are used. The COTS components are
not enough durable for space radiation environment. In
particular, a microprocessor embedded to OBC suffers aproblem of Single Event Latch-up (SEL). Horyu-2 was
the small-scale satellite developed by Kyushu Institute ofTechnology (KIT) and actually suffered many on orbit
anomalies due to SEL[1-2]. Therefore, the radiation test
is important for small-scale satellite using the COTS tocharacterize the radiation effect and to find most durable
COTS. However, a radiation test using an accelerator is
not readily available. Since 2012, KIT has been conducting radiation test using 252Cf for small-scale satellite. In
this report, recent radiation tests, using 252Cf, has beenreported. This ground experiment data was analyzed andcompared with the on-orbit data acquired from Horyu-2
in order to investigate the nature of anomaly.

Fig. 1 Test configuration

EXPERIMENTS: Figure 1 shows the schematic oftest configuration. A microprocessor, as device under test
(DUT), was set in a vacuum chamber. The pressure during the test was approximately 30 Pa. The model numberof microprocessor was HD64F36057FZJV and its plastic
cover was removed. The same model microprocessor was
mounted on Horyu-2. The radiation source of 252Cf was
mounted on XYZ stage. By changing a distance from thetest sample to 252Cf, radiation flux was calculated andcontrolled. DAQ and PC1 measured a voltage and currentof the microprocessor. PC2 monitored the operation of
microprocessor with RS232 communication. Just after
the SEL occurred each time, a reset command was sent to
the microprocessor. If the microprocessor was not recovered due to SEL, power was turned off.

Fig. 2 Probability of SEL occurrence for various fluxes
Table 1 Comparison between 252Cf test andon-orbit anomaly
252
Cf test
Orbit
Flux, 1/cm2/s
37
13
6.4
64
Simple average
3.4x106
19.3 42.2 86.3
time, s
Cross section of
1.3x10-6
1.3 1.8
1.8
SEL, x 10-3 cm2

RESULTS: 100 times SELs were observed and the time
between SELs was measured for each flux condition.
Figure 2 shows the probability distribution of a SEL occurrence with respect to time[3] at three different distances. As shown in Fig. 2, the time between SLEs is
increased with increasing of the flux and the probability
follows the Poisson distribution. Table 1 shows a SEL
occurrence time and the cross-section for ground experimental. On-orbit data from 2012 to 2015 is also shown. A
simple average SEL occurrence time was 1.2x107 sec (=139 days) from the orbit data. The cross-section derived

REFERENCES:[1] M. Cho et al., The Japan Society for Aeronautical andSpace Sciences, 12(0), 17-24, 2013.
[2] Y. Seri et al., SSC13-X-8, Small Satellite Conference,
August, 2013.
[3] T. Tomioka et al., Acta Astronautica, submitted for
publication.

採択課題番号 26053	
 カリフォルニウム線源を使用した衛星搭載用
通常採択
オンボードコンピュータに発生するシングルイベントの模擬試験および試
験方法の確立	 （九工大・先端）増井博一、冨岡孝裕、谷脇康洋、趙孟佑（京大・原子炉）高宮幸一	
 123CO5-9Instrumental Photon Activation Analysis of Geological and Cosmochemical Samples

N. Shirai, S. Sekimoto1, M. Ebihara

celerator at the Research Reactor Institute, Kyoto University. Electrons were accelerated by the linear accelerator to about 30 and 20 MeV. After irradiation (about 30
hours), samples were taken into new Al foil and measured at the Laboratory of Radioisotopes, Tokyo Metropolitan University. For comparative method, JB-1 wasused as reference standard.
RESULTS: Table 1 shows the interfering reactions andtheir contributions to nuclides produced by corresponding
reactions for activation with 20 MeV and 30 MeV electrons. As shown in Table 1, significant contributions
from interfering reactions were found in activation with
30 MeV electrons. Thus, determinations of Cr, Co and
Mn abundances need the correction of corresponding
interferences. As expected, contributions from interfering
reactions with 20 MeV electrons were lower than those inactivation with 30 MeV electrons.

Department of Chemistry, Tokyo Metropolitan University
Research Reactor Institute, Kyoto University

1

Normalized to reference values

INTRODUCTION: Bulk chemical compositions forterrestrial and cosmochemical materials are significantly
important to elucidate the formation, evolution processes
and magmatism of planetary bodies. Compared to geological samples, cosmochemical samples pose several
severe requirements to their analytical methods forchemical compositions. High sensitivity and accuracy foras many as elements as possible are required for analytical methods applied to such samples because of the limitation of sample amounts usable for analysis.
Non-destructive analysis for many elements is equallyfavorable. Nuclear analytical methods represented byprompt gamma-ray analysis (PGA), instrumental neutron
activation analysis (INAA) and instrumental photon activation analysis (IPAA) meet almost all these requirements. Among these nuclear analytical methods, INAA
has been commonly used as an analytical tool in comomochemistry for a long time, while PGA and IPAA havenot been very often applied to cosmochemical samples.
	  In IPAA, (γ,n) reaction is used for the determination ofelemental abundances which is an opposite reaction usedin INAA. Thus, IPAA could determine elemental abundances which cannot or hardly be determined by INAA.
Usually samples are irradiated by using 30MeV electronsin IPAA. However, corrections of interferences caused bysecondary nuclear reactions such (γ,p) and (γ,pn) arenecessary. Although the sensitivity obtained by activation
with 20MeV electrons are suppresses compared with theactivation with 30MeV electrons, activation with 20MeV
electron reduces the degree of such interference reactions.
In this study, we performed IPAA by using a linear electron accelerator at Kyoto University Research Reactor
Institute (KURRI) and compared the results obtained by
the activation with 20 MeV with those with 30 MeV.
EXPERIMENTS: Three GSJ standards materials namely JA-2 (andesite), JB-3 (basalt) and JR-1 (rhyolite) and
one cosmochemical sample (Allende meteorite) wereanalyzed by IPAA. Chemical reagent sample, Fe2O3
powder and Cr, Mn and Ni metals were also irradiated tocorrect the interference reactions. Samples and chemical
reagents were taken into a sample container (9 mmφ)
made of highly Al foil. Five to ten samples were stacked,
among which thin foil disk (9 mmφ) of Au as a monitor
of the intensity of photon are placed. Samples in a block
were put in a quartz tube. We used a linear electron ac-

1.2
1.1

JR-1

JA-2

JB-3

Allende

1
0.9
0.8
0.7
0.6
0.5
0.4

Figure 1. Our Mn values obtained by using 20 and 30 MeV electrons
are compared with the corresponding reference values. Solid andopen symbols represent that data are determined by using 30 and
20 MeV electrons, respectively.

	  A total of 17 elements (Ca, Sc, Ti, Cr, Mn, Fe, Co, Ni,
Zn, As, Rb, Y, Zr, Nb, Cs, Ba and Ce) were determinedin geological reference materials and the Allende meteorite. Our Cr and Mn values obtained from activation with
30 MeV electrons were different from literature values.
Our Mn values obtained by using 20 and 30 MeV electrons are compared with reference values in Figure 1. For
four samples, Mn values obtained by using 20 MeV electrons are consistent with reference values, while those byusing 30 MeV electron are lower than literature values.
Differences of Mn values in JB-3 and Allende between
30 and 20 MeV electrons are more remarkable than thosein JR-1 and JA-2. Fe/Mn ratios of JR-1, JA-2, JB-3 andAllende are 8.1, 52, 60 and 162, respectively. In consideration of Fe/Mn ratios, overcorrections of the interfering
reactions were responsible for these differences. For other elements, there were no differences between the two
sets of our values obtained from the activations with 20
and 30 MeV electrons, which were consistent with literature values.

Table 1. Interfering reaction and correction rate for interference.
Reaction used forInterfering
Correction rate
determination
reaction
30 MeV
20 MeV
52Cr(γ,n)51Cr
56Fe(γ,αn)51Cr
0.036 mgCr/gFe
59Co(γ,n)58Co
60Ni(γ,pn)58Co
3.7 mgCo/gNi
0.88
mgCo/gNi
55Mn(γ,n)54Mn
56Fe(γ,pn)54Mn
6.2 mgMn/gFe
0.1 mgMn/gFe	
 採択課題番号
26067	
 放射化分析による宇宙・地球化学的試料の元素組成の定量	 （	 (首都大学東京理工）白井直樹、海老原充（京大・原子炉）関本俊	
 

124

通常採択

CO5-10Decomposition of Perfluorooctane Sulfonate by Gamma Ray Irradiation

A. Hashiguchi, M. Yoneda, Y. Fujikawa1

pyl alcohol (IPA) and alkaline potassium persulfate
solutions. Both solutions were purged with nitrogengas before the irradiation. The use of persulfate wastested because the substance is a known radical initiator that produces sulfate radical throughS2O82-→2SO4-・reaction. As a control, ethanol (a radical
scavenger) spiked with PFOS was also irradiated. The
IPA and persulfate solution was subjected to solid phaseextraction by Oasis HLB (strongly hydrophilic and lypophilic, Waters) resin prior to determination of PFOS.
Direct photolysis of solid PFOS by gamma-ray was investigated by irradiation of a 20μL drop of PFOS (concentration: 1g/L-methanol), dried on a microscope slide,and covered with a cover glass.
Irradiation dose was estimated by ceric sulfate dosimeter
utilizing the reduction of Ce4+ to Ce3+ by the radiation, or
the calculation considering the distance and angle fromthe 60Co radiation source. Concentrations of PFOS in
sub-samples collected before and after the irradiation
were determined by UPLC-MS/MS (Waters).
RESULTS: Fig.1 shows the decrease in the numbers of
PFOS molecules after gamma-ray irradiation of the dried
residue of PFOS solution. The decrease of PFOS molecules was roughly proportional to the adsorbed dose. Interestingly, the rate of decrease was strongly dependent
on the dose rate,
3E+16
and was faster at
2.5E+16
0.7‐0.9 kGy/h y = ‐2E+14x + 2E+16
the higher dose rate.
R² = 0.8352
2E+16
Since the genera1.5E+16
y = ‐8E+15x + 2E+16
tion of radicals in
R² = 0.9346
1E+16
the dried residue is
5E+15
negligible, the de1.5 kGy/h0composition
of
0
10
20
30
kGy
PFOS is attributed
Fig. 1 Decomposition of dried PFOS residue with time (kGy)to photoexcitationof PFOS followed by its decomposition. It has been
known that upon irradiation with UV, perfluorooctanoic
acid (PFOA), one of the PFCs known for its refractoriness, was decomposed, and the mechanism of decomposition was ascribed to direct photolysis rather than toradical reaction [1]. On the other hand, the decompositionof PFOS by UV has not been found so far. The present
result indicates that high energy photon (1.16 and 1.33
MeV γ ray from 60Co in this case) was probably needed
to induce the direct photolysis of PFOS.
The decomposition of PFOS in ethanol was 30% (initially 2.3× 1015 molecules) after 42 kGy (dose rate 2.7
kGy/h) of irradiation. After 38 kGy (dose rate 0.67
kGy/h) of irradiation, only 6 % of PFOS was decomposed in alkaline persulfate, while in IPA, 85% of PFOS
was decomposed, due probably to the radical reactions.
REFERENCES:[1] R. R. Giri et al., Water Sci. & Technol., 63 (2011)276-282.

Graduate School of Engineering, Kyoto University
1
Research Reactor Institute, Kyoto University

採択課題番号 26074（京大・原子炉）藤川

PFOS molecules

INTRODUCTION:
Perfluoro compounds (PFCs),
characterized by high chemical and thermal stability,
have been widely used in the world as water and oil repellent, car wax and fire extinguisher, etc. Among various
PFCs, perfluorooctane sulfonate (PFOS), a linear perfluoroalkyl sulfonate with eight carbon-chain length, hasbeen noted for its high bioaccumulation potential to wildlife and persistence in the environment. Among the various environmental problems associated with this recalcitrant substance, we were most interested in development of a practical technology that could be used
to polish-up the wastewater containing PFOS.
Existing practical treatment methods for removal of
PFOS from sewage effluent or wastewater are membrane filtration (especially reverse osmosis), or adsorption using activated carbon. Use of these methods
has a figure of merit as they are already installed inmany treatment plants, and the operation and management protocols for various micro-pollutants are
fairly well established. On the other hand, PFOS is notdecomposed by these methods, only concentrated in
the reject or adsorbents. A technique that can decompose PFOS in the concentrate is needed.
Photo-assisted methods have been known to be effective for decomposition of pollutants in air and water.
The treatment is done either via direct photoexcitationof the pollutant or mediated processes involving highly
reactive radicals generated by photolysis. UV light iscommonly used for the technology, but for particularly
recalcitrant pollutants such as PCBs and chloro-fluoro
aliphatic carbons, γ ray irradiation has been proved tobe most effective. The OH radical, solvated electron,and radical or cation of isopropyl alcohol (added as asource of organic radicals), produced in the mediumby γ ray, degraded the pollutants through reductive
dehalogenation processes.
In our study, we irradiated the PFOS in various media
withγray to investigate the possibility of decomposition of PFOS via direct photolysis or radical reactions.
EXPERIMENTS: A 414 TBq (as of February, 2008)60
Co in γ ray irradiation facility in KURRI was used asa γ ray source. All the reagents used were Japan Industrial Standard reagent grade unless stated otherwise.
Known amount of PFOS powder purchased from
Wako Chemical Industry was dissolved in methanol(HPLC grade), and was used to spike alkaline isopro-

難分解性有機フッ素化合物のγ線照射・分解実験
陽子（京大院・工）橋口 亜由未、米田 稔

125

通常採択

CO6-1

D-serine Acting as Competitive Inhibitor on Tryptophanase

A. Shimada1, I. Otsuka1, N. Fujii2 and T. Saito2

ice to stop reaction. 200 μL of the reaction mixture wasfiltered through Amicon Ultra Centrifugal Filters cutting
more than MW 3000, immediately injected on a
Crownpack CR (+) Resolution HPLC resolution column
equilibrated with the degassed eluent through a Degasser, and eluted at a flow rate of 0.9 mL/min at room
temperature with an HPLC pump. L-Trp synthesis from
L-Ser was determined measuring with a CD-1595 detector. Ellipticity [θ] was monitored at λ = 230 nm with
the CD detector, represented in units of mdeg. Ellipticity of the eluent was set up to zero at a wavelength of λ =230 nm, so the peaks of L-Trp appeared on the positive
side.
RESULTS AND DISCUSSION: For kinetic analysis,
TPase activity on L-Trp synthesis was assayed in triplicate at the same substrate concentration, averaged. Lineweaver-Burk plots were drawn based on the leastsquares method. The reciprocal of rate constant (ordinate) versus the reciprocal of substrate concentration(abscissa) was plotted for each concentration of D-Ser,
depicting a typical competitive inhibition plot. Kinetic
constants were calculated from these double-reciprocalplots, and also an inhibition constant KI of D-Ser wasdetermined from their slopes. Km was 44 mM, Vm 2.2
×10-4 mM/s, kcat 0.48/s and KI 419 mM. D-Ser is a competitive inhibitor against TPase in L-Trp synthesis reaction from L-Ser and indole. Competitive inhibitor usuallyshares a highly structural resemblance with its substrate.
D-Ser stereostructure fits into the active site structure of
TPase, promptly binding there. Although D-Ser can bindwith the active site, D-Ser is not involved in L-Trp synthetic reaction. Perhaps D-Ser cannot form aldimine-bond with PLP at the first step of L-Trp synthesis.
However, our previous studies have reported that TPase
becomes active on D-Ser in the presence of triammonium phosphate (TAP) to make the enantioselectivity flexible. TAP is the most important among ammonium
phosphates because it gives TPase the highest activity on
D-Ser. The presence of TAP promotes a small conformational change to TPase to fit D-Ser partly into the catalytic site of the active site and help D-Ser to form theexternal aldimine bond with PLP. This subtle steric interaction, whose detail is still being investigated, are very
necessary to transform D-Ser from inhibitor into active
substrate. Future research will determine a metabolic
pathway of L-Trp synthesis from D-Ser, and also
demonstrate the formation of an aldimine bond between
amino group of D-Ser and PLP at the first step of thisreaction in the presence of TAP.

1

Sustainable Environmental Studies, Graduate School ofLife and Environment Sciences, University of Tsukuba
2
Research Reactor Institute, Kyoto University
INTRODUCTION: A historical riddle about chiralhomogeneity, the origin of L-dominant amino acids inbiological world, has intrigued scientists for many years,
though there has been no general consensus as yet to it.
Life could not been born without homochirality, that is
to say, no homochirality – no life. However, we cannot
imagine at all when and how the homochirality wasestablished on early earth. Amino acids are stereochemically too labile to retain their homochiral state in natural environment because racemization pressure is overwhelmingly strong, especially in aqueous solution. An
elaborate mechanism is necessary to put biologicalworld into homochirally-stable state. The homochiralityof contemporary biological world is fully guaranteed byenzyme enantioselectivity. Since the enzyme enantioselectivity has remained unclear, a deeper understandingof its mechanism is required to unravel all the riddle ofthe origin of homochirality. We have so far researched amechanism of tryptophanase (TPase) enantioselectivity,with the aim of answering this difficult problem. TPasedegrades L-tryptophan (L-Trp) by β-elimination reaction, and also synthesizes L-Trp from L-serine (L-Ser)and indole by β-replacement reaction by use of its absolute enantioselectivity. On the other hand, it is perfectly inert to D-tryptophan (D-Trp) and D-serine(D-Ser) at all. Additionally these D-amino acids inhibit
TPase in L-Trp degradation and L-Trp synthesis from
L-Ser. The present report describes to focus simply on
D-Ser acting on TPase as a competitive inhibitor.
EXPERIMENTAL: Generally speaking, D-amino acidworks as inactive or inhibitor against enzyme. D-Ser
completely has no reaction to TPase. When TPase synthesizes L-Trp from L-Ser and indole, D-Ser inhibits thesynthetic reaction. Since kinetic analysis was effective
to probe the interaction between D-Ser and TPase, we
analyzed D-Ser behavior against TPase in L-Trp synthesis in terms of it. For kinetics, reaction was conducted at 50 °C for 4 hr in Dry Thermo Unit DTU-1B with 0,0.1, 0.2, 0.3, 0.6, or 1 M of D-Ser added in reaction
mixtures that were prepared by combining the required
L-Ser (10-100 mM) with fixed apotryptophanase(apoTPase, 0.46 μM), indole (5.4 mM) and pyridoxal
5'-phosphate (PLP) concentrations (0.4 mM) in 500 μL
of 0.1 M potassium phosphate buffer (PB), adjusted to a
pH of 8.3. After 4hr, the reaction mixture was cool on

採択課題番号 26012 ガンマー線照射された酵素の立体構造変化による立体選択性への影響 通常採択
（筑波大・生命環境系）島田秋彦、大塚郁美（京大・原子炉) 藤井紀子、齋藤 毅
126CO6-2

Study of Localization Estimation of Abasic Sites in DNA Irradiated with
Ionizing Radiation

K. Akamatsu, N. Shikazono and T. Saito1

microliters of water was added to the residue. The fluorescence intensities were measured both at 449 nm (ex.
347 nm for AF350) and at 520 nm (ex. 460 nm for
AF488). After the measurement, the enzyme cocktail
containing DNase I and phosphodiesterase I was added
to the solution, followed by being incubated for 3 h at
37°C. E values were calculated from the donor intensity
before/after the digestion.

Irradiated Cell Analysis Research Group, Quantum Beam
Science Research Center, Japan Atomic Energy Agency(JAEA)
1
Research Reactor Institute, Kyoto University
INTRODUCTION:
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, e.g., around high-LET ionizing radiation
tracks. However, detail of the damage is not known. We
have already developed a method for estimating degreeof localization of abasic sites (APs) in DNA using Förster
resonance energy transfer (FRET). The FRET efficiency(E) was calculated using the donor fluorescence intensities before/after enzymatic digestion of the labeled
AP-DNA [1]. First, we have applied the method to 4He2+(2.0 MeV/u, LET: ~70 keV/m)- 12C5+ (0.37 MeV/u,
LET: ~760 keV/m)- and 60Co -irradiated DNA in thesolid state. The results showed that 12C5+ beam likely
produced close APs within a track. The apparent distancecalculated from the E value was approximately 17 basepairs [2]. This finding indicates that direct radiation effect of 12C5+ beam near the Bragg peak produces clustered DNA damage. We have recently applied the method
to DNA in a cell-mimetic radical scavenging condition[3,4]. Here, we show new results using 4He2+ beam and60
Co -rays.

RESULTS AND DISCUSSION:

Fig. 1. Relationship between AP average density and FRET
efficiency for He ion beam (●) and 60Co -rays (○). The solidline indicates a theoretical curve for randomly-distributed APs
in DNA.

As shown in Fig.1, there was no difference in
FRET efficiency (E) between the two radiation sources.
But interestingly, all data points were above the curvefor random distribution. This finding suggests that AP
distribution for the -rays as well as that for the He
beam is not completely random. This tendency is similar to the result using dry DNA as sample for irradiation[2]. A radiation “spur” on or nearby DNA might sometimes produces clustered damage. In any case,knowledge of AP distribution for 60Co -rays as a reference is quite important to study DNA damage by ionizing radiation. More data points and discussions will beneeded to elucidate the problem.

EXPERIMENTS:●Sample preparation and He beam irradiation
The plasmid DNA digested by Sma I was used (linear
form). The DNA was dissolved to be 0.1 g/L in 0.2 M
Tris-HCl buffer (pH 7.5) which is a cell-mimetic condition in relation to radical scavenging capacity. One hundred microliters of the DNA solution was transferred toan irradiation folder [2], and was irradiated with the4
He2+ beam (12.5 MeV/u, LET: ~19 keV/m; TIARA,
JAEA), and 60Co -rays (LET: ~0.2 keV/m; Kyoto
University Research Reactor Institute: KURRI) were also
used as a standard radiation source.

REFERENCES:[1] K. Akamatsu, N. Shikazono, Anal. Biochem. 433(2013) 171-180.
[2] K. Akamatsu, N. Shikazono, and T. Saito, Radiat.
Res. 183 (2015) 105-113.
[3] K. Akamatsu, N. Shikazono, and T. Saito, KURRI
Progress Report 2012 (2012) 256.
[4] K. Akamatsu, N. Shikazono, and T. Saito, KURRI
Progress Report 2012 (2013) 263.

●Preparation of fluorophore-labeled irradiated DNA andthe FRET observation
The irradiated DNA (10 L in water) and 10 L of
100 mM Tris-HCl (pH7.5) were mixed in a microtube.
Two microliters of a mixture containing AF350 (donor
fluorescent probe) and AF488 (acceptor one) with a given molar ratio was added to the DNA solution and was
incubated for 24 h at 35°C. The fluorophore-labeled
DNA was purified by precipitation by ethanol. Twenty

採択課題番号 26017 放射線誘発ＤＮＡ損傷スペクトルの線質依存性に関する研究（原子力機構・量子ビーム）赤松 憲、鹿園直哉（京大・原子炉）齊藤 毅
127

通常採択
共同通常

CO6-3The Effect of Boron Neutron Capture Therapy (BNCT) on
Anti-tumor Immune Response

Suzuki T.1, Horie K.1, Ogawa S.1, Wakamatsu E.1,
Abe R.1, Sakurai Y.2, and Ono K.2

Notably, unlike X ray irradiation, BNCT did not enhance anti-tumor immune response. Although additional immunization with peptide vaccination and CTLA4
blockade after BNCT lead to the induction of immune
response, this combination therapy could not achievetumor regression (Fig.2B and 2C). Our further interest
is why BNCT could not enhance anti-tumor immune response. To understand the anti-tumor immune response
during radiation therapy determines the effective combination with radiation therapy and immune therapy.

1

Recerch Institute of Biomedical Sciences,
Tokyo University of Science2
Research Reactor Institute, Kyoto University

INTRODUCTION: Boron neutron capture therapy(BNCT) is an attractive therapy for local tumor control in
the treatment of brain tumor, melanoma, and so on [1,2].
However, some important issues are remained: the tumor-specific accumulation of highly concentrated boron,
the real-time quantification of boron concentration in
local tumor tissues, and the prevention of re-growth andmetastasis of residual tumor cells after BNCT.
Recently, it was reported that some cancer immune therapies could achieved significant regression of tumor inclinical trials. To achieve successful tumor regression,in this study, we try to establish the combination treatments with BNCT and immunotherapy [3,4].
Results and Discussions:
The effect of BNCT on immune system
Using mouse model, we examined the effect of BNCTon the antigen specific immunological response.
C57BL/6 mice, which were subcutaneously administrated
with 250 mg/kg BPA, and then treated with thermal neutron irradiation (1 MW, 50min in the heavy water facilityof KUR). To assess the immune response, mice were
immunized with antigenson footpad, and the immunological response of T cells was assessed (Fig.1A). Although transient lymphopenia was observed after neutron
irradiation, the number of immune cells was restored at
11 days after treatment. Assessing IFN- production, theantigen specific immune response was comparable inneutron irradiated mice, compared with control mice (Fig.
1B), suggesting that antigen-specific immune response
could be induced even after neutron irradiation.
Anti-tumor immune response after BNCT
It was previously reported that local X ray radiotherapy lead to the augmentation of anti-tumor immune response via the induction of inflammation and immunological cell death in tumor site [5]. Hence, we examineanti-tumor immune response in hosts which received
BNCT or X ray radiotherapy. Mice were challenged
B16 melanoma cells on leg, and, BNCT or local X ray
irradiation (12Gy) therapy were performed around 10
days after tumor challenge. Fourteen days after radiation
therapy, immune response against tumor derived antigen
was assessed (Fig.2 A). As a result, similar to previous
reports, anti-tumor immune response was augmented byradiotherapy with X ray (data not shown).

REFERENCES:[1] M. Suzuki, et al. Int. J. Radiat. Oncol. Biol.
Phys. 58(3): 892-896, 2004.
[2] M. Suzuki, et al. Int. J. Radiat. Oncol. Biol.
Phys. 60(3): 920-927, 2004.
[3] Lifu Dengu et al., J. C. I., 124 (2), 687, 2014.
[4] M. A. Curran et al., PNAS, 107(9), 4275, 2010.
[5] Lionel A. et al., Nature Med., 13(9), 1050,2007

採択課題番号 26049 BNCT の免疫に与える影響と免疫療法による全身治療との併用の可能性 通常採択
東理大・生命研）安部 良、鈴木利宙、小川修平、若松 英、堀江和峰（京大・原子炉）櫻井良憲、
小野公二

128

CO6-4In situ Visualization of Boron in Plants Using Neutron Capture Radiography

M. Kobayashi and T. Kinouchi1

part and a circular region just inside the cortex, which are
the regions rich in vascular bundles. Boron as borate
diester is specifically bound to the rhamnogalacturonan II(RG-II) regions of pectin in cell wall, and the RG-II has
been shown to occur in all cells of the roots at the samedensity [3]. Thus the distribution of B within roots seems
distinct from that of its acceptor molecule.
Besides borate diesters bound to RG-II regions ofpectin, B in plants can occur as free boric acid as well,when the plants are amply fed with B [4]. The free boric
acid in shoots corresponds to B taken up as luxury absorption beyond the amount equivalent to that of the acceptor. Radish seedlings used in this study were grown in
the presence of enough amount of B, and hence they werelikely to contain both RG-II-bound and free boric acid.
At present, we are not sure to which fraction of B thesignals in radiography are ascribed. However, the observed pattern of pit distribution seems inconsistent withthose expected for bound B: since the acceptor RG-II
occurs ubiquitously and evenly within the root, the bound
B is also expected to occur uniformly. Taken together, we
think that the signal detected in this study probably camefrom soluble, free boric acid in root tissues.
Radish deficient in B sometimes accumulates a blue
pigment in the roots, which is called “Ao-aza” (blue spot)
symptom. Interestingly, the regions where the blue pigment (presumably anthocyanin) accumulates overlap withthose showing signals in this study. It is suggested thatcells in the regions may require higher supply of B thanthe others. In the vascular bundles occurs cambium,
which contains the cells actively propagating. Higher
supply of B may be necessary to support rapid cell proliferation in these tissues.
As the subject of future investigation, it is necessary
to make clear which fraction of B (cell wall-bound or freeboric acid) has been detected in this radiography. Growing plants under various B supply to prepare samples
with different content of free boric acid, then examining
the pit frequency would give useful information on this
aspect. In addition, increasing the sensitivity and resolution is also necessary. Optimizing the condition of neutron irradiation or alkaline etching would be useful tosolve these problems.

Graduate School of Agriculture, Kyoto University
Research Reactor Institute, Kyoto University

1

INTRODUCTION:
Boron (B) is an essential micronutrient for vascularplants, and its deficiency is one of the major constraints
on crop production worldwide [1]. Boron deficiency
causes various physiological disorders including an inhibition of the development of young leaves, necrosis oftissues inside tubers or tap roots, or failure in seed set.
The understanding of physiological function of B inplants has progressed greatly during the last few decades.
Boron as boric acid occurs in cell wall, and forms 1:2
borate-diol diester with specific regions of pectin [2]. The
diester bonds serve as the inter-chain bridges of pectin,
thereby stabilizes the cell wall structure. On the other
hand, the transport and distribution of B in plant remains
elusive, since no radioactive isotope with an appropriate
half-life is available for this element. Revealing a differential distribution of B within tissues, if any, may give us
clues to the demands for B of different cell types, hence
may contribute significantly to a better understanding of
the physiological role of B. Thus, in this study we havebeen trying to apply boron neutron capture radiography
to the in situ visualization of B in plant roots.
EXPERIMENTS:
Radish (Raphanus sativus L. sativus) seeds were germinated on vermiculite in a growth chamber with alight/dark regime of 18/6 h, 22°C, and 60% relative humidity. Seedlings with uniform size were transferred tosolution culture, which was maintained in the same
growth chamber. The nutrient solution contained B at
0.5ppm. At 10 days after transfer to solution culture, thetap roots were detached from the seedlings and fixed withglutaraldehyde. Fixed samples were embedded in OCT
compound (Tissue-Tek), frozen in liquid nitrogen, andsectioned at 8-µm thickness with freezing microtome.
The ultrathin sections were transferred onto CR-39 nuclear track detector. The bright-field image of the section
was taken at this point, to record the structure of tissue
examined. The CR-39 plate was then irradiated with neutron for 15 min using Tc-Pn facility at Kyoto University
Research Reactor Institute. The irradiated CR-39 plate
was etched in NaOH solution, and the resulting pits wereobserved under microscope.

REFERENCES:[1] V.M. Shorrocks, Plant Soil, 193 (1997) 121–148.
[2] M. Kobayashi et al., Plant Physiol., 110 (1996)
1017–1020.
[3] T. Matoh et al., Plant Cell Physiol., 39 (1998)
483–491.
[4] T. Matoh et al., Soil Sci. Plant Nutr., 47 (2001)
779–784.

RESULTS AND DISCUSSION:
When the image of pits generated by neutron irradiation was merged with the section image taken prior to theirradiation, the pits were distributed unevenly over thesection. Higher density of pits was found in the central	
 採択課題番号 26056	
 	 	
 中性子捕捉反応を利用した植物組織におけるホウ素動態の解析	 	  通常採択	 （京大・農）小林	  優（京大・原子炉）木野内忠稔	
 
	
 
129

CO6-5

Measurement of Transmittance Spectra of a Cryo-Sectioned Tissueof Brain Tumor C6 Model in the Sub-Terahertz Reagion-II

N. Miyoshi and T. Takahashi1
Department of Tumor Pathology, Faculty of Medicine,
University of Fukui
1
Research Reactor Institute, Kyoto University

A

INTRODUCTION: The LINAC (linear particle accelerator) technology in the millimeter and terahertz waves
had been unique and had been used as a coherent synchrotron light in the research reactor institute of Kyoto
university (KURRI) to observe the transmittance spectraof a sectioned tissue of raw brain tumor C6 model as acollaborate 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 wasestimated a longer relaxation time component of the induced electricity for water molecules [2-3] in the raw
tumor tissue for three years at the linear analysis.
We also estimated what kind of water molecules become
dominant in the viable and necrotic cancer regions by thedifferent measurement method as an aim of 2D mapping
study.

(2) Sample preparation: A cryo-sectioned (thickness=100m) tissue was prepared from the raw C6 glial tumor
model using a Cryo-section Maker (Leica) and wassealed sandwich-type with saran-wrap film (thickness=10m), under freezing condition (-20 C) before the measurements.
RESULTS: Large amount of spectroscopic data (morethan 1,000) for the 2D mapping data have been analyzed
to now, but the analysis was not finished to be reported as
the imaging of each water components.
REFERENCES:[1] Phillip C. Ashuworth, et. al., Optics Express, 17(14):12444-12454 (2009).
[2] Toshiko Fukasawa, et al., Phys. Rev. Let., 95: 197802(2005).
[3] Hiroyuki Yada, et al., Chem. Phys. Let., 464: 166-170(2008).

EXPERIMENTS: (1) Instrument of Near-field intera-hertz region: The photograph of the instrument was
shown in Figure 1. Mark-A: Pre-probe Wiston cone;50-10mm diameter, Length= 60mm; the irradiate diameter= 0.775mm; The concentrate light probe (diameter)= 3mm. The instrument was developed by Dr. T.
Takahashi in KURRI [Figure-1] for the 2D mapping
analysis.

採択課題番号 26072

テラヘルツ近接場分光装置を用いた実験脳腫瘍モデル組織のイメージング分光（福井大・医）三好憲雄（京大・原子炉）高橋俊晴
130

通常採択

CO6-6

Design and Synthesis of New Drugs for Boron Neutron Capture Therapy andBoron Magnetic Resonance Imaging

S. Aoki1, Y. Nishiura1, T. Tanaka1, Y. Hisamatsu1, Y.
Sawamoto1, Rikita Araki2, Takaomi Saido3, T. Suzuki4, K.
Horie4, Ryo Abe4, S. Masunaga5, K. Natsuko5, Y. Sakurai5, and K. Ono5

[3].
These results prompted us to design and synthesize its
analog (3) having an icosahedral carborane (o-carborane)
unit that consist 10 borons and 2 carbons as a potent carrier of boron cluster to the cancer cells. It was found that
this molecule is transferred into cancer cells more effectively than 1. Moreover, we have discovered that theo-carborane unit of 3 decomposes in the presence ofd-block metals in aqueous solution at neutral pH and release more than 4 molecules of B(OH)3 [4]. Besides,
o-carborane analog 4 having methanol unit instead ofcyclen also undergoes the full decomposition to release10 B(OH)3. This change was successfully detected on 11B
NMR and MRI. Because the chemical and physical properties of 10B and 11B are almost identical, these probes
should be useful not only for BNCT, but also for the determination of the distribution of boron-containing drugs
in the bodies and of the biorelevant d-block metals.

1

Faculty of Pharmaceutical Sciences, Tokyo University of
Science2
Bruker Biospin K. K.
3

RIKEN Brain Science Institute4

Research Institute of Biomedical Sciences, Tokyo University of Science
5
Research Reactor Institute, Kyoto University

INTRODUCTION: Boron neutron capture therapy(BNCT) is one of powerful therapies for local tumor control in the treatment of brain tumor, melanoma, and so on[1]. However, some important issues are remained for theachievement of successful tumor regression: the tumor-specific accumulation of highly concentrated boron,
the real-time quantification of boron concentration in
local tumor tissues, and the prevention of re-growth andmetastasis of residual tumor cells after BNCT. In thisstudy, we have designed and synthesized new boron
compounds appended with macrocyclic tetramines suchas cyclen (1,4,7,10-tetraaminocyclododecane) for BNCT
and B-MRI [2]. It was expected that boron clusters suchas icosahedral carboranes would be transferred to living
cells due to the dicationic properties of cyclen part at
neutral pH.
Icosahedral carboranes are boron clusters composedwith 10 boron atoms and 2 carbon atoms which exhibit aremarkable thermal and chemical stability. In this maniscript, we reported first example of full deboranation reaction of o-carborane catalyzed by copper(II) ion. Initially,
we examined the deboronation reaction of ortho-carborane-cyclen in aqueous solution in the presenceof various d-block metals such as Cu2+, Zn2+, Fe2+, Ni2+
and Co2+.

Fig 1. Design and decomposition reaction ofboronylated compounds
REFERENCES:[1] a) R. F. Barth et al., Clin. Cancer Res., 11 (2005)
3987-4002. b) R. F. Barth et al. Rad. Oncol. 7 (2012)
146-166.
[2] a) G. W. Kalbalka, et al. J. Neuro-Oncol. 33 (1997)
153-161. b) P. Bendel, NMR in Biomed. 18 (2005) 74-82.
[3] M. Kitamura et al., Inorg. Chem. 50 (2011)
11568-11580.
[4] Y. Nishiura et al., Manuscript in preparation.

EXPERIMENTS and RESULTS:
Synthesis of boron compound based on
Boron is one of ultratrace elements in living systems.
Previously, we have designed and synthesized boron-pendant cyclic tetraamine 1 for the in-cell 11B NMR(nuclear magnetic resonance) or MRI (magnetic resonance imaging) for the detection of metal in living systems and eventually for the use in BNCT. It was reported
that the C-B bond is hydrolyzed upon complexation withd-block metals to giveone molecule of boric acid
(B(OH)3) as well as zinc complex of N-benzylcyclen 2

がん組織に集積する含ホウ素化合物の設計・合成と
共同通常
通常採択
腫瘍への集積のホウ素 MRI に向けた基礎検討（東理大・薬学部）青木 伸、西浦由紀子、田中智博、久松洋介、澤本泰宏（ブルカーバイオスピン）荒木力太（理研）西道 隆臣（東理大・生命研）鈴木利宙、堀江和峰、
安部良（京大・原子炉）増永慎一郎、近藤夏子、櫻井良憲、小野公二
採択課題番号 26077

131

CO7-1

Evaluation of Boron-containig Rare Earth Oxides Nanoparticles as an Agentfor Boron Neutron Capture Therapy	 T. Nagasaki, R. Kawasaki, S, Iizuka, H. Yukawa, Y. Tsujimoto, M. Kirihata1, K. Tomita2, K. Katagiri3, K. Ono4, S.
Masunaga4, and Y. Sakurai4
Graduate School of Engineering, Osaka City University,
1
BNCT Research Center, Osaka Prefecture University,
2
School of Science, Tokai University
3
Institute of Engineering, Hiroshima University
4
Research Reactor Institute, Kyoto University

Fig. 1 TEM images of boron-containing rare earth oxide
nanoparticles; (A) SmBO3; (B) GdBO3; (C) YBO3.

INTRODUCTION: Boron Neutron Capture Therapy(BNCT) is a highly selective cancer therapy that can target single tumor cell without causing excessive radiation
damage around normal cells. The success of BNCT depends on the delivery that 10B compounds accumulate
effectively inside the tumor cells. Clinically, boronophenylalanine (BPA) and borocaptate sodium (BSH) arecurrently used for BNCT as boron delivery agents but
these agents have some disadvantages on accumulation or
selectivity toward tumor tissue. In addition, the efficacy
of boron neutron capture reaction is suppressed due tolow neutron fluence. In this study, in order to improve theefficiency of neutron capture reaction, we used boron
containing rare earth oxides nanoparticle (SmBO3,
GdBO3, YBO3). When their diameter is suitable sizes,
these nanoparticles could be significantly accumulated intumor tissue with EPR effect. Moreover, the particle
doped with europium can possess the fluorescence. This
fluorescent nanoparticles are expected as novel borondelivery drugs that can diagnose and treat cancer simultaneously and efficiently.

Fig. 2 Comparison of the antitumor efficacy withrare earth oxides/chondroitin sulfate complex.

cokinetics by using BALB/c mice bearing colon26 murine carcinoma. The highest boron concentration of
YBO3 nanoparticle in tumor tissue was observed at 6hours after administration by i.p. Then, BNCT was performed on tumor-bearing mice. Two hundred µl of
nanoparticle solution (concentration of 10B: 132 ppm
with SmBO3 and GdBO3, 88 ppm with YBO3) were injected by i.p. before 6 hr of neutron irradiation at Kyoto
University Research Reactor (1 MW, 90 min, 4.1×1012
neutron/cm2). By irradiation, YBO3 nanoparticle showedstrongest antitumor effect among used rare earth oxides
nanoparticles (Fig 2).
As the nanoparticle of the rare earth oxide could contain huge boron atoms per particle, it can deliver efficiently a lot of boron toward tumor tissue with EPR effect. Especially, As yttrium had no shield effect toward
neutron, YBO3 showed highest BNCT effect. Therefore,
this YBO3 nanoparticle is promising toward next generation BNCT.

EXPERIMENTS: The cell colorectal cancer line colon26 were used in this study. Boron containing rareearth oxides nanoparticles were synthesized by homogeneous precipitation method. Cationic nanoparticle arecoated with anionic chondroitin sulfate (XBO3/ch, X: Sm,
Gd, Y). Boron concentration was estimated by ICP-AES.
Cytotoxicity of nanoparticle was estimated by WST assay.
RESULTS AND DISCUSSION: The TEM images
showed that the particle haves spherical shape with relatively homogenous distribution and its diameter is about
100 nm (Fig. 1). The result indicates that its size is suita	 blefor EPR effect. Moreover, we evaluated its pharma-

REFERENCE:[1] K. Fujita et al., J. Ceram. Soc. Jpn., 98, 991(1990).

採択課題番号 26005	
 含ホウ素希土類酸化物のＢＮＣＴ薬剤としての評価	 （阪市大院・工）長﨑	
 
	
  	
  	
  	
  	
  	
  	
  	
  	
  	
  健、河崎	  陸、飯塚俊輔、湯川寛子、辻本裕貴、櫻本昌士

	
 

通常採択	
 

（阪府大・21研究機構）切畑光統（東海大・理）冨田恒之（広大・工）片桐清文（大阪府大BNCTｾﾝﾀｰ）服部能英（京大・原子炉）小野公二、増永慎一郎、櫻井良憲、田中浩基
	
 

132

CO7-2

In vivo Evaluation of Gd-DTPA-incorporated Calcium Phosphate Nanoparticles
as Neutron Capture Therapy Agent

N. Dewi1, P. Mi2,3, H. Yanagie1,4,5, Y. Sakurai4, H.
Cabral2 , N. Nishiyama3, K. Kataoka2,6, Y. Sakurai7, H.
Tanaka7, M. Suzuki7, S. Masunaga7, K. Ono7, H.
Takahashi1,4

mice group with higher concentration of gadolinium.
Nevertheless, further investigation is necessary toconfirm the reason of moderate tumor growth
suppression in multiple-injected mice group.

1

Dept of Nuclear Engineering & Management, Univ ofTokyo, 2Bioengineering Dept, Univ of Tokyo, 3Polymer
chemistry division, Chemical Resource Laboratory,
Tokyo Institute of Technology, 4Cooperative Unit ofMedicine & Engineering, Univ of Tokyo Hospital, 5DeptofInnovative
Cancer
Therapeutics,
Meiji
Pharmaceutical University, 6Materials Engineering
Dept, The University of Tokyo, 7Research Reactor
Institute, Kyoto University
INTRODUCTION: Gadolinium-157 has been getting
attention as alternative for neutron capture therapy(NCT) agent because of its high thermal neutron crosssection (255 000 barns), which the highest among all
stable elements. However, compared to short range
secondary particles produced after neutron captureby 10B isotope currently used for clinical trial of NCT,
gadolinium neutron capture reaction (Gd-NCR) results
in release of gamma rays, which reduce the localization
effect of the treatment, which on the other side isincreasing the possible additional effect if Gd-157 isaccumulated to a bulk tumor cluster.
In this work, we performed in vivo evaluation oftumor growth suppression on multiple-injections GdDTPA/CaP nanoparticles mice as continued work fromprevious evaluation on single-injected group [1].

Figure 1. Experimental procedure for multipleinjected tumor-bearing mice.

EXPERIMENTS: In vivo evaluation was performedon colon-26 tumor-bearing mice irradiated for 60
minutes at nuclear reactor facility of Kyoto University
Research Reactor Institute with average neutron fluenceof 1.8 × 1012 n/cm2. Experimental procedure formultiple-injected groups is illustrated in Fig. 1.
Antitumor effect was evaluated on the basis of thechange in tumor growth and survival rate of the mice.
RESULTS: Higher gadolinium accumulation in tumor
site was successfully achieved for multiple injections of
Gd-DTPA/CaP nanoparticles, up to more than threetimes compared to single injection (data not shown).
There was no acute toxicity in the treated mice,indicating the promising possibility of Gd-DTPA/CaP as
Gd-NCT agent. However, we could not observe better
tumor growth suppression after GdNCT treatment,
which indicates the possibility of neutron depression on

Figure 2. Tumor growth suppression comparison
between single-injected and multiple-injected GdDTPA/CaP.
REFERENCES:[1] Dewi N et al., KURRI Progress Report (2013) CO7-21.
[2] Dewi N et al., Biomed & Pharmacother (2013) 67:451-7.
[3] Mi P, et al.: J Cont. Release (2014) 174:63-7.

採択課題番号 26014 中性子捕捉療法法の一般外科領域癌への展開に向けた基礎的研究

通常採択（東大・原子力国際専攻）高橋浩之、柳衛宏宣、Novriana Dewi（東大・獣医）柳川将志、飯塚智也（東大・心臓外科）櫻井由里子、毛利きくえ （京大・原子炉）小野公二、増永慎一郎、鈴木 実、櫻井良憲

133CO7-3Development of a Phantom for Estimation of Beam Quality in BNCT
tron dose is increased to almost 50% greater than a purewater phantom for which the fast neutron dose contribution is at most 10%.

Y. Sakurai, T. Takata, N. Fujimoto, H. Tanaka, N. Kondo,
Y. Nakagawa, M. Suzuki
Research Reactor Institute, Kyoto University
INTRODUCTION: After the restart of the operation of
Kyoto University Reactor (KUR) in May 2010, 235 clinical studies of boron neutron capture therapy (BNCT)
have already been carried out as of May 2015 [1]. Also,
the BNCT clinical trial using Cyclotron-based BNCT
Epi-thermal Neutron Source (C-BENS) started in November 2012 [2]. In the while, the research and development into several types of accelerator-based irradiation
systems are underway by several research groups in theworld at present time. With this situation in mind, it isimportant that the physical and biological estimations fordose quantity and quality are performed consistently
among several irradiation fields, and that the equivalencyof BNCT is guaranteed, even across BNCT systems. The
individuality of irradiation fields can stand out for the
beam-quality characteristic of the incident fast neutrons,
such as the mixing ratio and neutron energy spectrum.
The aim of this research is the development of the phantom made of specialized materials for the estimation of
the beam quality. In 2014, a feasibility study on the estimation of relative biological effectiveness (RBE) for fastneutrons, based on the simulation and experimental dataobtained for the proto-type “beam-quality estimation
phantom”.

Fig. 1. Depth distributions of total dose rate and its
breakdown in the pure water phantom.

METHODS: As a beam-quality estimation phantom, aphantom of 10% LiOH solution with 95%-enriched Li-6
was prepared [3]. The simulated thermal and fast neutron
fluxes were converted into absorbed dose rates in normal
tissue [4]. The composition for normal tissue was assumed to be H:11.1, C:12.7, N:2.0, O:74.2 in weight percent [5], and the density was assumed to be 1.0 g/cm3.
The operation power of KUR was 1 MW.

Fig. 2. Depth distributions of total dose rate and its
breakdown in the 10%-6LiOH phantom.

RESULTS: Figures 1 and 2 show the depth distributionsof the total dose rate and its breakdown in the pure water
phantom and the 10%-6LiOH phantom, respectively. In
the pure water phantom as shown in Fig. 1, the contribution of gamma rays is dominant and it becomes larger at
depth, over the interior of the phantom. In the
10%-6LiOH phantom as shown in Fig. 2, the thermal
neutron dose rate decreases to below almost one-thirtiethof the fast neutron dose rate. In addition, the gamma-ray
dose rate decreases to the same order as the fast neutron
dose rate.

REFERENCES:[1] Y. Sakurai et al., Nucl. Instr. Meth. A 453 (2000)
569-596.
[2] H. Tanaka et al., Nucl. Instr. Meth. B 267 (2009)
1970-1977.
[3] Y. Sakurai et al., Proc. 14th Int. Congr. Neutron Capture Therapy (Comision Nacional de Energia Atomica) (2010) 254-256.
[4] R.S. Caswell et al., Radiat. Res. 83 (1980) 217-254.
[5] W.S. Synder et al., Report of the Task Group on Reference Man (Pergamon Press, Oxford, 1975).

CONCLUSION: The condition for a larger contributionof fast neutron dose is realized in the 10%-6LiOH phantom. It can be expected that the accuracy for RBE estimations in biological experiments would improve using
the 10%-6LiOH phantom as the contribution of fast neu-

採択課題番号 26034
ＢＮＣＴのための線質評価ファントムの開発（京大・原子炉）櫻井良憲、田中浩基、藤本 望、近藤夏子、仲川洋介、鈴木
134

通常採択
実

CO7-4

A Fundamental Experiment for the Measure Against the Activation of the
Irradiation-room Concrete at BNCT Facility

Y. Sakurai, T. Takata, K. Kimura1, H. Tanaka, K. Takamiyahydrogen density was smaller. From the comparison forthe latter activity, it was found that the generation of thesecondary thermal neutrons was decreased to almost one
fifth for the resin with B4C. In the while, the activity,
namely the thermal neutron intensity, was increased according to the thickness. This is due to the influence forthe secondary thermal neutrons generated in the concrete.

Research Reactor Institute, Kyoto University
Fujita Corporation

1

INTRODUCTION: At present time, the research anddevelopment into several types of accelerator-based neutron sources for boron neutron capture therapy (BNCT)
are underway by several research groups in the world,with Cyclotron-based BNCT Epi-thermal Neutron Source(C-BENS) at the head of the list [1]. In near future,
BNCT using the accelerator-based neutron sources may
be carried out at several places in the world. Unlike thefacilities for radiation therapy and charged-particle therapy, the neutron yield is larger at BNCT facility. Then,the activation of concrete, which is a main structure of
the irradiation room, is larger. The use of low-activation
concrete is prefer in the viewpoints of the decrease of
exposure under the work in the irradiation room, the decommissioning of the irradiation room, etc.. This research is intended to perform the characteristic estimation
for low-activation concrete and confirm its usability at
BNCT facility. In 2014, a fundamental experiment for themeasure against the activation of concrete using an
Am-Be neutron source was performed, because the operation of Kyoto University Reactor (KUR) was limited.

CONCLUSION: From this experiment, it was realizedagain that the measure for the low activation of concreteitself, namely the development of low-activation concrete
was important, even if the measure against the activation
was performed using the neutron shield. The estimations
for the important characteristics of low-activation concrete are planned, such as short-life activation, long-life
activation, the shielding effect for neutrons and gamma
rays, the generation of the secondary gamma rays, etc.,
when the KUR operation is restarted.

METHODS: A characteristic estimation was performed
for the measure against the activation using a neutron
shield for a commercially available normal concrete. A
resin containing B4C, which is under development, wasused as a neutron shield. This shield weakens neutron
intensity to reach the concrete, by that high-energy neutrons are moderated by hydrogen in the resin and thermal
neutrons are absorbed by boron in B4C. As nine resin
sheets of 10-cm side, 10-cm long and 2-mm thickness
were stacked on the concrete surface, the shielding performance against the Am-Be neutron source was estimated by foil activation method. Indium foil was used as
an activation foil. The shielding characteristic for fastneutrons was estimated by the activity change forIn-113(n,n’)In-113m reaction, and the generating characteristic for the secondary thermal neutrons was estimatedby the activity change for In-115(n,γ)In-116m reaction.

Fig. 1. Activity changes dependent on the thickness
for the resin without B4C.

RESULTS: Figure 1 shows the activity changes dependent on the thickness for the resin without B4C. Figure 2 shows the activity changes dependent on the thickness for the resin with B4C. In these figures, the activity
changes for In-113(n,n’)In-113m and In-115(n,γ)In-116m are drawn. From the comparison for the former activity, it was found that the shielding effect for fastneutrons was a little smaller for the resin with B4C, as its

Fig. 2. Activity changes dependent on the thickness
for the resin with B4C.
REFERENCES:[1] H. Tanaka et al., Nucl. Instr. Meth. B 267 (2009)
1970-1977.

採択課題番号 26035
ＢＮＣＴ施設用低放射化コンクリートの特性評価（京大・原子炉）櫻井良憲、田中浩基、高宮幸一
135

通常採択

CO7-5

Radiosensitizing effect of purinergic antagonists on thedamage of melanoma by BNCT

M. Tsukimoto1, N. Mori1, K. Nishino1, T. Suzuki1, K.
Horie1, K. Tanamachi1, D. Kitahara1, N. Kondo2, S. Masunaga2, Y. Sakurai2, R. Abe1
12

Tokyo University of Sciences
Research Reactor Institute, Kyoto University

INTRODUCTION: Radiation exposure causes DNA
damage, and DNA repair systems are essential to rescue
damaged cells. Release of extracellular nucleotides, suchas ATP, from cells plays a role in signaling via P2 receptors. We have reported that autocrine/paracrine signaling
through P2X7-dependent ATP release and activation of
P2Y6 and P2Y12 receptors serves to amplify the cellularresponse to DNA damage caused by γ-irradiation [1-3].
BNCT is one of the new radiation therapy that mainlyuse α-ray derive from 10B(n,α)7Li reaction. 10B is delivered to the cell as 10B-bromophenylalanine (BPA). Since
it is known that melanoma tend to incorporate phenylalanine, 10B-BPA is well incorporated into melanoma.
γ-ray is low-LET radiation, and BNCT is high-LET radiation. γ-Irradiation causes DNA damage by indirect
action effect, which is mediated by reactive oxygen species. However, BNCT causes DNA damage by direct
action. It is known that direct action effect is stronger
than indirect action effect. Further, BNCT can irradiate
cells from inside of the cell.
Recently, we have showed involvement of P2
receptors in DNA damage repair after γ-ray irradiation in
A549 cells [2]. However, it has not yet been clear the
involvement of P2 receptors in BNCT-induced DNA
damage response. If the activation of P2X7, P2Y6, orP2Y12 receptor are involved in BNCT-induced DNA
damage response, the antagonists of these P2 receptors
enhance cytotoxicity of cancer cells by BNCT. Here, weinvestigated the radiosensitizing effect of P2 receptor
antagonist on BNCT-induced DNA damage response andcytotoxicity.

EXPERIMENTS:
Mouse melanoma B16 cells wereincubated with 1 mM 10B-BPA and P2Y12 receptor
antagonist clopidogrel. B16 cells were irradiated with
γ-rays and thermal neutron beams from a nuclear reactor(Kyoto University Research Reactor Institute;1 MW) atroom temperature for a suitable time. After irradiation,
the cells were incubated in humidified atmosphere of 5%
CO2 in air at 37 oC.
The irradiated cells were fixed in 4% paraformaldehyde
in PBS for 10 min at room temperature and permeabilized in 0.1% Triton X-100 for 5 min on ice. After incu-

bation in blocking buffer (10% FBS in PBS) for 1 h, thefixed cells were incubated with primary antibody against
γH2AX for 24 h at 4 oC and with 2nd antibody conjugatedwith FITC for 1 h. Counterstaining with Hoechst 33258
was used to verify the location and integrity of nuclei.
Fluorescence images were obtained with a laser scanningconfocal microscopy.
On the other hand, cell viability of irradiated cells
were measured by colony formation assay. 1.0 x 103
cells were seeded in a 100 mm dish. After incubation for
1 week, the cells were stained with 0.5% crystal violet.
Colonies containing more than 50 cells were counted.
RESULTS: First, we tested the effect of BNCT on cell
survival rate by the colony formation assay. Survival
fraction of BNCT group decreased compared with groupof γ-irradiated cells. In addition, the cytotoxic effect of
BNCT was enhanced by pre-treatment with clopidogrel(Fig.1A). Next, we tested DNA damage response after
BNCT by analyzing γH2AX focus formation. Formationof γH2AX foci that remain for 48hr was increased by
BNCT. The BNCT-induced increase of γH2AX foci was
suppressed by pretreatment with clopidogrel (Fig. 1B).
From these results, it was suggested that P2Y12 receptor participated in DNA damage repair caused by BNCT.
(A)

(B)

Fig.1 The effect of clopidogrel on BNCT-induced
DNAdamage responce
REFERENCES:[1] Tsukimoto M. et al., Radiat. Res. (2010) 173(3):298-309.
[2] Nishimaki N et al., DNA Repair (Amst). (2012) 11(8): 657-65.
[3] Ide S. et al., J Toxicol Sci. (2014) 39(1):15-23.

採択課題番号 26061	
 	
 	
 DNA 鎖損傷修復抑制効果をもつプリン受容体阻害薬を用いた
通常採択
BNCTによる抗癌増強効果	
 	 	
 （東京理科大・薬）月本光俊、森夏樹、西野圭祐、棚町圭祐、北原大輔、（東京理科大・生命研）
鈴木利宙、堀江	  和峰（京大・原子炉）櫻井良憲、増永慎一郎、近藤夏子	
 136

CO7-6 Feasibility Study for Establishing QA Method for Hospital- and Reactor-based BNCTTPR20,10 of a medical linac and the energy dependence ofthe film to gamma-rays, Monte Carlo simulation(BEAMnrc ver. 4.2.4. [6]) was used, and comparison of
PDDs between measurement and simulation with the
BEAMnrc were performed. Therefore, contribution of the
gamma-rays was subtracted from the output of the film.

S. Nakamura1, 2, A. Urushiyama2, T. Nishio3, C. Kurokawa4, A. Wakita1, M. Ito1, M. Munechika5, H. Okamoto1, Y.
Sakurai6, H. Tanaka6, N. Fujimoto6 and J. Itami1
1

Department of Radiation Oncology, National Cancer
Center2
Rikkyo University
3
Graduate School of Biomedical & Health Sciences, Hiroshima University
4
Department of Radiology, Juntendo University
5
Department of Human Sciences, Tokyo Metropolitan
University
6
Research Reactor Institute, Kyoto University

RESULTS: The comparison of PDDs between measurement and simulation was performed with a medical
linac of 4, 6, 10, and 15 MV photon beam in National
Cancer Center (NCC), Tokyo, Japan. The difference of
those beams between the measurement and the simulation
was within 0.59%. The relationship between TPR20,10 andthe calculated energy dependence which was normalized
in the value of 6MV photon beam in NCC. With using
those relationship and BEAMnrc, energy dependence ofthe film in the medical linac in Juntendo University andthat in KURR was 1.002±0.003, and 0.986±0.002, respectively. Outputs of the TLD after irradiation in KURR
were multiplied by a value of the ratio of energy dependence in KURR to that in Juntendo University, and themultiplied values were subtracted from the dose with thefilm. The relationship between the thermal neutron fluence and the dose with the film was shown in Fig. 1. The
thermal neutron fluence was proportional to the dose withthe film.

INTRODUCTION: In general, boron neutron capture
therapy (BNCT) is currently performed using a nuclear
reactor [1], [2]. Recent researches [3], [4], [5] have madepossible to acquire an adequate amount of neutrons byaccelerator and hospital-based accelerator-BNCT hascome into reality. Therefore, National Cancer Center,
Tokyo, Japan, is planning to install an accelerator-based
BNCT system. Hospital-based accelerator-BNCT system
has a lot of advantages. For example, there is no need tomove a patient to the reactor. However, the hospital-based system also has disadvantages. In the hospital-based BNCT system, with compared with the reactor-based BNCT system, the measurement for a beam of
BNCT is asked for the simplified method because thehospital-based system is restricted by an area of the institute. The purpose of this study is to establish the QA
method for hospital-based BNCT.
EXPERIMENTS: In order to measure easily the neutron
beam, new film was developed. The new film consistedof thermos luminescence phosphor. After exposure of theradiation, the output of the film with heated was red by
CCD. Signal intensity was measured as the amount oflilght. The relationship of the film between the signal anddoses were acquired with 6 MV photon beam of a medical linac in Juntendo University, Tokyo, Japan. The relationship between the signal and neutron fluence was analyzed in this study because the signal was evaluated as
the dose. The experiment of neutron irradiation was performed in Kyoto University Research Reactor (KURR).
In order to evaluate the film, the thermal neutron fluence
was measured with the film and a gold foil, and theseresults were compared. However, the beam of the KURR
contained both neutrons and gamma-rays. Therefore, thedose from gamma-rays was measured with the thermoluminescence dosimter (TLD) since the film also had
sensitivity to photons. The contribution from the gamma-rays to the film was considered by the result of the
TLD. In order to evaluate a relationship between theFig. 1. The relationship between the dose with thefilm and thermal neutron fluence.
REFERENCES:[1] K. Nakai et al., Appl. Radiat. Isotopes., 69(12):1790-1792; (2011)[2] S. Masunaga et al., Br. J. Radiol., 85(1011): 249-258;(2012)[3] S. Kamada et al., Appl. Radiat. Isotopes., 88:
195-197; (2014)[4] H. Kumada et al., Appl. Radiat. Isotopes., 88:
211-215; (2014)[5] H. Tanaka et al., Appl. Radiat. Isotopes., 69:
1642-1645; (2014)[6] DWO Rogers et al., Med. Phys., 22: 503-524; (1995)

共同通常
通常採択
採択課題番号 26068
BNCT 照射場の QA/QC に関する基礎研究（国立がんセ・放治）中村 哲志、岡本 裕之、脇田 明尚、伊藤 昌司、伊丹 純、（広島大院・
医歯薬）西尾 禎治、（首都大・人間）宗近 正義、（京大・原子炉）櫻井 良憲、田中 浩基、藤
本 望

137

CO9-1

Stability of Caprolactam Resin against γ-Ray Irradiation in HNO3

T. Nishida1, M. Nogami1, and N. Sato25-membered ring would be necessary to obtain plural
neighboring C=O groups under the present irradiation
condition.

1

Graduate School of Science and Engineering Research,
Kinki University
2
Research Reactor Institute, Kyoto University
INTRODUCTION: We have previously reported thatthe property of structure change in a cyclic monoamide
resin consisting of poly-N-vinyl-ε-caprolactam (VEC)
with a 7-membered ring by γ-ray irradiation in HNO3 isdifferent from that in polyvinylpolypyrrolidone (PVPP),
another cyclic monoamide resin with a 5-memberedring[1]. Namely, while relatively stable plural neighboring C=O groups (structure (a) in Fig. 1) were introduced for PVPP[2], such neighboring C=O groups were
not observed for VEC. In this study, to clarify the moredetailed degradation property of VEC, other irradiatedsamples were prepared and analyzed. Water-soluble
N-methyl-ε-caprolactam (MEC) was also irradiated in
HNO3 to evaluate the stability of VEC quantitatively.
N

O

VEC

Fig.2. Expected major route of change in chemical structure of VEC by γ-ray irradiation in HNO3
In a 1H NMR spectrum, neat MEC showed four signals; (A)3.4，(B)2.9, (C)2.4, (D)1.6 ppm, respectively.
The calculated residual ratios are shown in Fig. 3 together with the relationship between the position of hydrogenin the structure of MEC and that of the signal. The residual ratios calculated from (A), (B) and (D) show anearly identical trend, where the residual ratios decreaselinearly with an increase in dose, and ca. 50 % and 75 %are decomposed at 1 and 2 MGy, respectively. On theother hand, the residual ratio calculated from (C) is foundhigher than the three other systems, which would be because the signal (C) overlaps with that of degraded compounds. The dependence of residual ratio of N-butylpyrrolidone (NBP), one of the water-soluble 5-memberedrings, under the irradiation in 6 M HNO3 on dose is difference from that of MEC. Namely, the decrease in theresidual ratio of NBP decreased steeply and then gently[3]. As the result, comparing the stability of MEC
with that of NBP, the residual ratio of MEC is higher thanthat of NBP at less than ca. 0.6 MGy, and vice versa at
more than 0.6 MGy.

N
COOH

N

OH
O

H

HO

PVPP

COOH

H

N

HN

O
HOOC

O

O

NH

HO

O

(a)

Succinic acid

NH2

COOH
COOH

Fig. 1. Expected major route of change in chemical
structure of PVPP by γ-ray irradiation in
HNO3[2].
EXPERIMENTS: γ-Ray irradiation to VEC was carriedout similarly to the earlier study (max. 1.5 MGy)[1].
For the sample of MEC, a solution containing 1 mol/dm3(= M) MEC and 6 M HNO3 was prepared. The sample
solution was put in a Pyrex tube and irradiated by the60
Co source at max. 8.8 kGy/h up to 2.1 MGy at room
temperature under ambient atmosphere. Irradiated samples were analyzed by 1H and 13C NMR. DMSO-d6
containing a known weight of TMS which is a standard
material was used as the NMR solvent. The residual
ratio of MEC was calculated by the area ratio of eachsignal with that of TMS.

Rssidual ratio/%

100

(B)

75
50
25
0
0.0

(A)

A
B
C
D
0.5

(C)

(D)
1.0

1.5

2.0

2.5

(D) (D)

Dose/MGy

RESULTS: A crystal was observed from the supernatantobtained from the irradiated VEC. The crystal was
identified as succinic acid by 13C NMR analysis. The
structure change in VEC is expected from the result asshown in Fig. 2, which suggests that the major route ofchange in chemical structure of VEC is basically identicalto that of PVPP and that the resulting dicarboxylic acids
differ corresponding to the number of carbon in the cyclicmonoamides. The scheme is consistent with the abovementioned fact that plural neighboring C=O groups were
not observed for VEC. These facts also imply that a

Fig.3. Dependence of residual ratio of MEC on dose.
REFERENCES:[1] T. Nishida et al., KURRI Progress Report 2013(2014) 295.
[2] M. Nogami et al., J. Radioanal. Nucl. Chem., 296(2013) 423-427.
[3] M. Nogami, et al., Sci. China Chem., 55 (2012)
1739-1745.

採択課題番号 26013 アクチニルイオン配位性アミド化合物の耐ガンマ線性に関する研究 通常採択
（近大・理工）西田哲大、野上雅伸（京大・原子炉）佐藤信浩

138

CO9-2

Search for Ultraviolet Photons from Precipitated 229mTh Samples

Y. Yasuda, Y. Kasamatsu, Y. Shigekawa, T. Ohtsuki1, K.
Takamiya1, A. Shinohara

RESULTS: In the case of the hydroxide and fluoride
samples of 229mTh grown for about 2 h, the count rates ofphotons were almost the same with those of the background. In contrast, for the 229mTh samples grown forabout 13 h, the photon emissions decaying for time weredetected and the half-lives were about 1 h for hydroxideand 3 h for fluoride. For example, the result for the229m
ThF4 sample grown for about 13 h is shown in Fig. 2.
These decaying photon emissions, however, did not seemto be the simple decay curve. In addition, if the half-livesof 229mTh were several hours, the photon emissions are
expected to be observed for the samples grown for 2 h.
Therefore, these photons might derive from the Cherenkov radiation induced by the decay of daughter nuclides
such as Bi or Pb. To clarify the origin of these photons,
we plan to purify 229mTh before measurement.

Graduate School of Science, Osaka University
Research Reactor Institute, Kyoto University

1

INTRODUCTION: The first excited state of 229Th
lies in extremely low energy level. The excitation energy
was reported to be 7.8 ± 0.5 eV [1]. This energy corresponds to vacuum ultraviolet light, and it is expected thatthe decay rate of 229mTh varies drastically depending on
their chemical forms [2]. Furthermore, chemical conditions can affect the decay mode of 229mTh (internal conversion and/or gamma ray transition). It is also expectedthat 229mTh can be applied to a nuclear clock which has
about two orders higher precision than the most precise
optical clock [3]. Hence, many studies have been performed to observe the decay of 229mTh, especially on
photon detection. However, there are not clear results
directly observing the decay. It is important to observe
the photons emitted from the 229mTh on various chemical
conditions to understand the decay property of the state.
This report describes the results of photon detection forthe several samples containing 229mTh with different
chemical forms: hydroxide and fluoride.

REFERENCES:[1] B. R. Beck et al., LLNL-PROC-415170 (2009).
[2] E. V. Tkalya et al., Phys. Rev. C 61, 064308 (2000).
[3] E. Peik et al., Europhys. Lett. 61, 181 (2003).

EXPERIMENTS: Thorium-229m was separated fromthe mother nuclide 233U by using anion-exchange method.
About 200 mg of 233U, containing less than 1 ppm of 232U,
was adsorbed on the anion-exchange resin (Dowex 1×8,
200-400 mesh, 2.5 mL). Five-milliliters of 9 M HCl solution was poured into the column several times to remove
229m
Th and the daughter nuclides. After 229mTh was grownin the column for a certain time: about 2 or 13 h, 5 mL of
9 M HCl solution was passed through the column to elute
229m
Th. To prepare the hydroxide samples, 20 µL aliquotof samarium standard solution was added and then aqueous NH3 was added to the eluent until the solution became basic. When the fluoride samples were prepared, 30µL aliquot of samarium standard solution and 2 mL of
HF solution were added to the eluent and the solution
was stirred for 2 min. Thorium-229m was coprecipitatedwith samarium as hydroxide or fluoride form. Each precipitate was collected on a polypropylene filter and heated to dryness.
Setup for photon detection is schematically illustrated inFig. 1. To measure vacuum ultraviolet ray from 229mTh
samples, we used a photomultiplier tube (PMT) for photon counting, Hamamatsu R6837, which detects 4-10 eV
photons with higher than 10 percent quantum efficiency.
Signals from PMT were amplified with the pre-AMP and
PM-AMP. Noise was cut with the discriminator, and thesignal data were accumulated in the multichannel analyzer.

Fig. 1. Schematics of the experimental setup for photon
detection.

Fig. 2. Count rate of photons for the 229mThF4 sample
grown for about 13 h.

229m
採択課題番号 26079
Th の紫外光及び電子測定
即時採択（大阪大院・理）安田勇輝、笠松良崇、重河優大、篠原厚（京大・原子炉）大槻勤、高宮幸一

139CO10-1

Study on the Behavior of Cs and Sr in Soil as Waste

M. Yoneda, 1, S. Fukutani2, M. Ikegami2, Y. Shimada1, Y.
Matsui1

3.5 !

1

Graduate School of Engineering, Kyoto University
2
Research Reactor Institute, Kyoto University

3.0 !

INTRODUCTION: After the accident of Fukushima
Daiichi nuclear power plant, decontamination work has
been carried out. Soil containing radioactive materials
such as Cs is present in the decontamination waste. It isnecessary to understand the behavior of radioactive substances in case of the incineration of waste. Therefore, inthis study, the dissolution test was carried out using
heat-treated soils containing Cs and Sr. Moreover, mostof these kind of experiments are carried out using muchhigher concentration of stable isotope compared to theactual pollution concentration. Therefore, the differenceof the results between in case of using high concentration
stable isotope and in case of using actual level concentration of radioisotope is investigated.

stable Cs!

elution rate

2.5 !

Cs-134!

2.0 !
1.5 !
1.0 !
0.5 !
0.0 !
0!

200!

400!

600!

800!

heating temperature

EXPERIMENTS: The soil of the A1 layer of coniferous trees forest of Iwate University Takizawa practiceforest was used for the experiment. 10 g of the soil of theA1 layer was taken and made into samples with additionof 5 µg of stable Cs (mainly Cs-133) and Sr (mainly
Sr-88) or 1250Bq of Cs -134 and Sr -85. 10 ml of distilled water was added to each soil sample, and eachsample was dried for 20 hours in 45 degree Celsius temperature. Then, each sample was heated at 100, 200, 300,
400, 500, and 600 degrees Celsius using muffle furnacefor one hour, and then they were let cool off naturally.
After the addition of distilled water to each heat treatedsample at solid-liquid ratio 1:10, they were shaken for six
hours and centrifuged for ten minutes. Finally, supernatant liquid of them were filtered using 0.45 µm filter andthe filtrates were measured by Pure Ge semiconductor
detector or ICP-MS.

Fig. 1 Relation of elution rate of Cs and heating temperature.

350!
300!

elution rate

250!

RESULTS: The results are shown in Fig. 1 and Fig. 2.
Fig. 1 showed that the elution rate of Cs decreased withincreasing heat treatment temperature, and that there wasalmost no difference between in case of using high concentration stable isotope and in case of using actual level
concentration of radioisotope is investigated. It is highly
possible that less Cs in the decontamination waste containing soil is eluted in the environment because of the
fixation of Cs in soil by the heat treatment. Fig. 2 showedthat the elution rate of Sr increased with increasing theheat treatment temperature. Because of high concentration of background stable Sr, the elusion rates for stable
Sr and radioactive Sr cannot be compared. However,their tendencies with the temperature of heat treatment
are almost same.

200!

stable Sr!

150!

Sr-85!

100!
50!
0!
0!

200!
400!
600!
heating temperature

800!

Fig. 2 Relation of elution rate of Sr and heating temperature.

	
 採択課題番号 26075	
 土壌・廃棄物中での Cs および Sr の挙動に関する研究（京大・原子炉）福谷哲、池上麻衣子（京大院・工）米田稔、島田洋子、松井康人	
 
140

通常採択

	
 

CO11-1

Study of Intense Terahertz Light Source Based on
Superimposing Backward Coherent Diffraction Radiation

N. Sei and T. Takahashi1

Al u mi n u m fo i lmi rro r
Ab so r b e r

T i wi n d o w

Research Institute for Measurement and Analytical Instrumentation, National Institute of Advanced Industrial
Science and Technology
1
Research Reactor Institute, Kyoto University

Aluminum plate

El e c t r o nb e am

D i f f r ac t i o n e l e m e n t s

INTRODUCTION: A relativistic electron beam with ashort pulse width is suitable for generating intense terahertz (THz) light. We have proposed to develop amonochromatic THz light source based on a superimposing coherent diffraction radiation (CDR). We observed a sign of the superimposing CDR to the electron-beam trajectory with an L-band electron linac at the
Kyoto University Research Reactor Institute (KURRI-LINAC) [1]. However, the forward CDR interferedwith coherent transition radiation (CTR) generated at a Ti
window. It is difficult to evaluate the spectrum of thesuperimposing CDR quantitatively. The CDR is also
emitted behind the electron-beam trajectory. The powerof the backward CDR in the THz region is as strong asthat of the forward CDR. Then, we have conducted experiments about superimposing backward CDR.

Accelerator room
Shield wallu r t i n - Pu p l e t t t y p e
Experimental room M
i n t erfero met er

B ac kwar d
CDR

Schematic layout of the CDR experiment.

Fig. 1

CDR intensity [ a.u. ]1.0

EXPERIMENTS: When a relativistic electron-beamemits radiation by a periodic structure, the resonancewavelength in laboratory system is influenced by Lorentz
transformation. The resonance wavelength  is given by

l 1
(1)
    cos  ,n  

Al u mi n u m
c o l l i m at o r

1sheet2sheets
8sheets
16sheets

0.8

0.6

0.4

0.2

0.0
1




2

3

4

5

6

7

Wavelength [mm]Fig. 2where l, , and n are the period of the diffraction elements, the velocity of the electron divided by the speed oflight, and the order of higher harmonics, respectively.
The symbol  is the angle between the electron-beam
trajectory and the direction of the CDR. It becomes  inthe case of the backward CDR. Thus, the wavelength offundamental harmonic of the backward CDR is the sameas the double of the period of diffraction elements.
Figure 1 shows the schematic layout of the experimental setup of the backward CDR at KURRI-LINAC.
Because an aluminum foil mirror was set to transport the
backward CDR to the experimental room, it did not interfere with a CTR beam emitted from the Ti window. A
thin aluminum plate, which was located behind the diffraction elements, prevented backward CTR generated by
the vacuum chamber interfering with the backward CDR.
An aluminum collimator with a diameter of 17.5 mm was
located in front of the aluminum foil mirror. The distance
between the aluminum foil mirror and the entrance of thediffraction elements was 120 mm, and the inner diameterof the diffraction elements was 30 mm.
Figure 2 shows spectra of the CDR when the periodof the diffraction elements was 19 mm. It is noted that theSpectra of the CDR generated by the diffrac-tion elements.
CDR intensity at wavelength around 3.8 mm, which was
double of the period, increased as the number of the diffraction elements increased. However, the intensity did
not increase for the number of the diffraction elements
exponentially, so that the ratio that the CDR was superimposing was low. Because the bunch length of the electron beam was approximately 10 ps, the interaction
length of the superimposing CDR was not longer than theresonance wavelength, and the ratio would become small
as the number was larger.
RESULTS:We observed backward CDR generated
by diffraction elements with a period of 19mm. Althoughan enhancement of the CDR intensity was observed at thefundamental resonance wavelength, the ratio that the
CDR was superimposing was low. We will plan to use
diffraction elements which had a shorter period.
Reference:[1] N. Sei and T. Takahashi, KURRI Progress Report2013 (2014) 222.

通常採択
採択課題番号 26004 重畳的コヒーレント回折放射による高強度テラヘルツ光源 共同通常（産総研）清 紀弘（京大・原子炉）高橋 俊晴
141CO11-2

The XEP-e (eXtremely High Energy Plasma/ Particle Sensor for Electron)of the ERG Satellite

N. Higashio, H. Matsumoto, T. Takahashi1, N. Abe1
Japan Aerospace Exploration Agency
1
Research Reactor Institute, Kyoto University
INTRODUCTION: It is well known that satellites andastronauts are always endangered in space due to plasma,
radiation particles, neutral particles, ultraviolet rays/Xrays and meteoroids/debris. Since we have to support
JAXA’s projects to keep them safe from the space environment, our group has been researching the radiation
environment of space for more than 20 years. Now weare developing a sensor for the ERG (Energization andRadiation in Geospace) satellite. The purpose of the ERG
satellite is to investigate the mechanism of radiation belts.
It is well known that the energetic electron flux varies
during geomagnetic disturbance and especially the relativistic electrons in the outer radiation belt change. However, the data of the electron (10eV - 20MeV) in radiation
belt is not enough. The ERG satellite consists of four
instrument parts, Plasma/Particle (PPE), geomagnetic
field (MGF), Plasma wave (PWE) and electric field(PWE). Before using KURRI-LINAC (Kyoto University),
we couldn’t calibrate our sensor over 2 MeV electrons.

Fig. 2. XEP-e

Fig. 3.

Principle of the XEP-e

We need very low count rate beam (100~1000cps), so
we tried to make this beam by using the XEP-e (EM) lastyear. And this year we calibrate the XEP-e(Flight Model).
As shown in Fig. 4, the data that is got in KURRI-LINAC and simulation data (GEANT4) were very similar between 5MeV and 14MeV. It shows KURRI-LINAC
can make very low count rate beam.

Fig. 1. ERG satellite
EXPERIMENTS: Our sensor that name is XEP-e(Extremely High-Energy Plasma/Particle Sensor forElectron) is one of the PPE. The XEP-e observes
400keV~20MeV electrons and has five solid-state silicondetectors (SSDs) and a high-Z scintillator (GSO). The
XEP-e is Fig.2. The first SSD discriminate between electron and other particles. And The 2~5 SSDs and a high-Z
scintillator detect its energy. Fig. 3.
We use KURRI-LINAC (Kyoto University) to calibrate
its energy (2MeV~20MeV electron). We also use ouraccelerator in Tsukuba space center under 2MeV electron.

Fig. 4.

Incident energy vs Loss energy of the XEP-e(energy range: 5MeV~14MeV)RESULTS:
There haven’t been facilities that can make very low
count rate beam over 2MeV in Japan. But now KURRILINAC (Kyoto University) can only make low count rate
and monochrome beam between 5MeV and 14MeV.

採択課題番号26071
ERG 衛星搭載超高エネルギー電子観測装置(XEP-e)校正試験
通常採択(宇宙航空研究開発機構)東尾奈々、松本晴久、高島健（京大・原子炉）高橋俊晴、阿部尚也（明星電気㈱）江口信次郎、尾本敬信、(㈱ファムサイエンス)藤井雅之
142

CO12-1

Precise Determination of Br in ABS Resin by
Instrumental Neutron Activation Analysis

T. Miura1, R. Okumura2, Y. Iinuma2, S. Sekimoto2, K.
Takamiya212National Metrology Institute of Japan, AIST
Research Reactor Institute, Kyoto University

INTRODUCTION: National Metrology Institute of Japan is responsible for developing certified reference materials (CRMs) 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 CRMs. Recently, neutron activation
analysis (NAA) using comparator standard is recognized
as a potential primary ratio method [1]. Despite thepotential of NAA as primary ratio method, the evaluationof the measurement uncertainty is required in any analysis. In general, there are three main components of uncertainty in NAA, 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 theflux monitor can correct the neutron flux variation using
the count rate of the known amount of the monitor nuclide, it does 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].
In this paper, we presented that notable capability of internal standardization in NAA for determination of Br inacrylonitrile butadiene styrene copolymer (ABS) resin
as a candidate CRM.

One hundred mg of the ABS resin samples was used for
Br analysis. The Au solution was added to the samples
before neutron irradiation. The neutron irradiations
were performed by KUR (Kyoto University Research
Reactor) TCPn (thermal neutron flux: 8.0 x 1010 cm-2s-1)
for 6 h. The γ ray measurement system consisted of a
Canberra GC4070-7500 Ge detector and a Laboratory
Equipment Corporation MCA600.
RESULTS: It was found that the 198Au sensitivity(cps/µg) varied according to the sample position in theirradiation capsule. The relative standard deviation of the
198
Au sensitivity (cps/µg) was 3.8 %. The uncertainty
related to the neutron flux homogeneity significantly
contributes to the overall uncertainty, if an internal standard is not applied. The amount of Br in the ABS resin
sample was determined by calibration curve method using internal standardization. The linearity of calibration
curve was improved by internal standard. The relative
standard uncertainty related to the calibration curve linearity was improved to 0.36 % to 0.87 %. The analyticalresults of Br in BCR-681 certified reference material ofpolyethylene resin by proposed method were in excellent
agreement with the certified value only using internal
standard.
The analytical results of Br in ABS resin sample byproposed method was 575 mg/kg±8.0 mg/kg (n=8). The
relative expanded uncertainty (k=2) was 1.4 %.

EXPERIMENTS: The ABS resin candidate CRM wasproduced by a mixing machine. The calibration solution of Br was prepared from NMIJ primary standard
solutions. The Au solution for the internal standard for
Br was prepared from a high purity metal. The calibration solutions contained Br and Au as internal standard.
REFERENCES:[1] R.Greenberg, P. Bode, E. De Nardi Fernandes,
Spectrochim. Acta B, 66 (2011) 193-241.
[2] T. Miura, K.Chiba, T. Kuroiwa, T. Narukawa, A.Hioki,
H. Matsue, Talanta, 82 (2010) 1143-1148.

採択課題番号 26008 内標準法を併用した中性子放射化分析法の高精度化に関する研究 通常採択
共同通常
（産総研・計測標準）三浦勉（京大・原子炉）関本俊、奥村良、飯沼勇人、高宮幸一

143CO12-2

Thickness and Density of Adsorbed Additive Layer onto Metal Surface
under Rolling Friction Evaluated by Means of Neutron Reflectometry

T. Hirayama, N. Yamashita1, S. Akimoto1, M. Fujimori1,
T. Matsuoka1, M. Hino2 and T. Oda2
Dept. of Mechanical Engineering, Doshisha University
Dept. of Mechanical Engineering, Doshisha University
2
Research Reactor Institute, Kyoto University
1

INTRODUCTION:
Tribology is one of academic
disciplines covering friction, wear and lubrication inengineering for a lot of industrial applications such as
bearings, gears, engine pistons in car and so on.
Formation of adsorbed additive layer on metal substrates
has attracted attention as an effective way to reduce
friction. There are a lot of studies investigating therelationship between the kind of additives and their
tribological properties, but the formation process of theadsorbed layer is still unknown. On these backgrounds,
this study investigated the formation and desorption
process of adsorbed additive layer onto metal surface bymeans of attenuated total refection infrared spectroscopy(ATR-IR) and neutron reflectometry (NR) with time slice
mode.
EXPERIMENTS:
Thin copper film was deposited
onto silicon wafer as target substrate for the study.
Poly-alpha-olefin and palmitic acid were selected as baseoil and oiliness additive, respectively. The timedependences of IR absorbance profiles and neutronreflectivity profiles are shown in Figs. 1 and 2. We cansee that the IR peaks from COO bonds gradually grown
up after the injection of base oil with oiliness additive.
On the other hand, the neuron reflectivity profiles did notchange regardless of time. These results indicated that thephysisorption of oiliness additive molecules was quickly
completed and the chemisorption was graduallyproceeded. To investigate the effect of rolling friction, we
designed the sample holders with rolling friction
mechanism for ATR-IR and NR. The obtained results areshown in Figs. 3 and 4. The IR profiles showed thedesorption of additive layer, but the NR profiles did notchange even after the rolling friction.

Fig. 1.

Fig. 2. Time dependence of neutron reflectivity profiles
obtained by SOFIA at BL16 in J-PARC MLF

Fig. 3.

Time dependence of IR absorbance peaks after
rolling friction

Fig. 4.

Time dependence of NR profiles after rolling
friction

CONCLUSIOINS: The additive molecules made thecondensed layer around the top surface by physisorption,and they gradually reacted by chemisorption. The rolling
friction process pealed the adsorbed additive molecules
off from the surface temporarily, but the layer was
quickly repaired. ATR-IR and NR were quite effective to
see the adsorption and desorption processes withseparating ‘physisorption’ and ‘chemisorption’.

Time dependence of IR absorbance peaks

採択課題番号 26020

中性子反射率法による摺動条件下における
表面添加剤吸着層の厚み・密度測定（同志社・理工）平山朋子、山下直輝、秋元翔太、藤森慎、松岡敬（京大・原子炉） 日野正裕、小田達郎
144

通常採択
共同通常

CO12-3

Characteristic Mesurement of Neutron Detector for Fukushima Debris

M. Kureta1, M. Komeda1, K. Takamiya2
1

Japan Atomic Energy Agency
Research Reactor Institute, Kyoto University

2

INTRODUCTION:
New hybrid detector called B-10+ detector has beendeveloped by GE Reuter-Stokes. The detector is what
combines B-10 lined proportional counter with He-3
counter. A big feature of B-10+ detector is reducing costs
while the performance doesn’t decrease much. We havedeveloped NDA system against the Fukushima debris,and then we are considering applying the B-10+ detector
instead of He-3 detector that has been most popular for
general NDA systems. The original experiment plan at
KUR was twice experiments at the B-4 port, and once
experiment with high gamma ray and neutron flux at thearea under the core. We could carry out the first experiment in 2014. In the experiment using the B-4 port, we
obtained fundamental data of B-10 detector such as thepulse shape and plateau.
EXPERIMENTS:
The B-10+ detector is 100cm in length. And the gaspressure including He-3 is approximately 1 atm. Threetypes of amplifiers were used. A current amplifier andcharge amplifier are developed by our group, and anotheris a charge amplifier from PDT Inc. He-3 detector (4 atm)
was also used in order to compare detection efficiency
with B-10+ detector. The high voltage power supply was
ORTEC 556H, DC supply was KIKUSUI PDM-3, andcounter was ORTEC 872.

Fig.1 Plateau measurements of B-10+ detector withthree kinds of amplifiers

1V
0.4μs

RESULTS:As shown Fig.1, the current amplifier and charge amplifier caused pile-up, which was also observed on an
oscilloscope. Therefore we measured neutron flux
through an absorber, the plateau region was observed
clearly. Due to the limited machine time, data of the attenuated flux was not obtained by using a current amplifier, and data after the plateau region was not done. Somemeasurements by He-3 were carried out. As an easy reference, measurement result by He-3 detector indicatesthat B-10+ detector has 40% detection efficiency of He-3
detector. Fig.2 shows a pulse from a charge amplifier onan oscilloscope. The width was approximately 1 μs thatwas the same degree as using He-3 at another measurement. Fig.3 shows an output spectra for a B-10+ detector.
A sharp peak of He-3 was not observed. The reason isconsidered that the effect of the He-3 gas is not stronger
than the lined B-10 since the amount of He-3 gas is reduced. We will investigate characteristics of B-10+ detector in high gamma ray field as future work. After that,
we will try experiments applying B-10+ detectors to
NDA system.

採択課題番号 26022（原子力機構）呉田

Fig.2 A pulse from B-10+ detector using acharge amplifierFig.3 B-10+ detector spectrum using a charge
amplifier

福島溶融デブリ測定用中性子検出器の特性評価研究
昌俊、米田 政夫（京大・原子炉）高宮 幸一

145

通常採択

CO12-4

Evaluation of Multiwire-type Two-Dimensional Neutron Detector
with Individual Line Readout

K. Toh, K. Soyama, T. Nakamura, M. Hino1, and T. Oda2
J-PARC Center, Japan Atomic Energy Agency
1
Research Reactor Institute, Kyoto University
2
Graduate School of Science, Kyoto University
INTRODUCTION: Multiwire-type two-dimensional
neutron detectors using helium-3 gas are widely used inneutron scattering experiment facilities because of theirhigh detection efficiency, low gamma-ray sensitivity, andexcellent long-term stability. We have developed anadvanced multiwire-type two-dimensional neutron
detector system without compromising the otherwise
excellent performance of the conventional detector [1, 2].
A short response time and better spatial resolution can beobtained in this system by using an individual line
readout method. Additionally, optical devices have beendeveloped and incorporated in the system forlong-distance signal transmission and insulation between
the detector heads and the signal processing circuits. In
this present study, we performed neutron irradiation
experiments at KUR.

Fig. Image of collimated neutron beam with size of 1 x 1
mm2.
Normalized signal (arb. unit)

101

EXPERIMENTS: The multiwire element, which isdeveloped for individual line readout, has 128 anodewires, 128 cathode wires for the y-axis, 128 cathodestrips for the x-axis, and a wire/strip pitch of 1 mm. The
amplifier-shaper-discriminator boards have a total of 256
channels to process each cathode signal line.
Field-programmable gate array based digital signal
processing and digital signal encoding are used to
calculate signal position with a sampling frequency of
106 MHz. Dedicated optical signal transmission devices
are designed to use multimode optical fibers at awavelength of 850 nm. List-mode data with the x- andy-positions and the time of flight are recorded using adata acquisition system (MPA-3, Fast Comtec). Neutron
irradiation is performed using a neutron beam line CN3 at
the KUR.

100
10-1
10-2
10-3
10-4
10-5

0

20

40
60
80
Position (mm)

100

120

Fig. 2 one dimensional response at peak position.
106
Measured signal (cps)105

RESULTS: Fig. 1 shows a typical response when a 1.0
× 1.0 mm2 neutron beam is irradiated on the detector, andthe response at the peak position onto the x- axis isshown in Fig. 2. As seen in Fig. 2, there are somebackground signals. It is considered that these signals
arise from neutron scattered by the beam line, thecollimator, the window and the fill gas. Fig. 3 shows thereactor power dependence to the measured counts of thedeveloped detector system. The developed detector
showed a linear response up to the full power, 5 MW, of
KUR reactor and the counting rate at 5 MW wasapproximately 2.1 x 105 cps.

2.1 x 105 cps

104
103
102
101
100
10-1
10-5

5 MW

10-4

10-3

10-2

10-1

Reactor power (MW)

100

101

Fig. 3 Measured counts of developed system under
neutron irradiation as a function of KUR reactor power.
REFERENCES:[1] K. Toh et al., Nucl. Instr. and Meth., 726 (2013)
169-174.
[2] K. Toh et al., J. Phys.: Conf. Ser. 528 (2014) 012045.

採択課題番号 26042
個別信号読み出し MWPC 二次元中性子検出器の特性評価（原子力機構）藤 健太郎、曽山 和彦、中村 龍也（京大・原子炉）日野 正裕（京大院・工）小田 達郎
146

通常採択

CO12-5

Development of Neutron Resonance Densitometry for
Nuclear Material Quantification in Melted Fuel

F. Kitatani1, H. Tsuchiya1, M. Koizumi, J. Takamine1, J.
Hori2, M. Sano2, K. Takahasi2, K. Nakajima2, and H.
Unesaki2
1
2

and the abscissa time interval after neutron pulse generations. The dips in the spectra around 192 and 102 ns areresonances of 183W at 7.64 eV and 27.0 eV, respectively.
Since the origin of the spectra is relevant to the beginningof electron pulse injection, the ends of the dips come lateras the electron pulse width increases. The dip at 27.0 eV
is not clearly seen with 4-s electron pulse width.

Research Group for Nuclear Sensing, JAEA
Research Reactor Institute, Kyoto University

INTRODUCTION: Neutron Resonance Densitometry(NRD) [1, 2] is an assay technique of nuclear materials inparticle-formed debris that contains various nuclides,
such as of structural materials and the others. It is a combination of two techniques: Neutron Resonance Transmission Analysis (NRTA) [3], and Neutron ResonanceCapture Analysis (NRCA) [4] or Prompt Gamma-ray
Analysis (PGA). Containing nuclides in a sample are
identified by NRCA/PGA. The information of
NRCA/PGA is used in NRTA analysis to quantify nuclear
material isotopes. A neutron time of flight (TOF) method
is used in NRD measurements. A facility consisting of aneutron source, neutron flight paths, and detectors, isrequired. One of the distinctive features is utilization of ashort flight path; this increases the neutron beam strength,
and reduces construction cost in a practical applications.
On the other hand, that reduces resolving power in TOF
measurements, and increases neutron background. Inorder to investigate the effect of neutron flight length, we
carried out NRTA experiments with a short neutron flightpath constructed at the Kyoto University Research Reactor Institute - Linear Accelerator (KURRI-LINAC).

SUMMARY: In measurements of NRD, the quantity of
the nuclear materials is determined from NRTA spectra in
the neutron energy range of less than 30 eV [1, 2]. At
KURRI-LINAC, we have examined NRTA with a 7-m
flight path. The resonance dips of 183W at 27 eV wassuccessfully observed with an electron pulse width lessthan 2 μs. This indicates the applicability ofshort-flight-path TOF system to nuclear material quantification. The importance of the pulse width of neutron
beam should be noted. Both simulation studies and experiments are expected for realistic design of a TOF facility of nuclear material quantification.

EXPERIMENTS: Experiments were carried out with a
7.5-m flight path. The experimental room and the neutron
source were separated by 2-m-thick concrete wall. A
2-m-long neutron transport tube was installed in the experimental room as shown in Fig. 1. The center of it wasan Al vacuum chamber, the cavity of which was 200 mm
in diameter; both sides were shielded by 2-mm-thick Al
plates. The chamber was surrounded by 5-mm-thick
B4C-doped silicone rubber (B4C 40%). The outside of therubber was high density polyethylene plates (460 x 460mm). The neutron beam was collimated to be 50 mm indiameter in front of the transport tube. A 6Li scintillation
detector (Saint-Gobain GS20; 100 x 100 x 10 mm) wasused to measure transmission neutrons. The incident neutron flux was monitored by a BF3 neutron detector placednear the exit of the concrete wall.
Sample and filter plates (100 x 100 mm) were placed in
front of the transport tube: In (0.2 mm), Ag (0.25 mm), W(0.5 mm), and Pb (10 mm). The neutron pulse width wascontrolled by the pulse width of the LINAC electron
beams, which were 500 ns, 2 μs and 4 μs.

Fig. 1. A neutron transport tube. A neutron detector wasplaced on the table.

Fig. 2. TOF neutron transmission spectra. The baselines are adjusted, and the curves are added for the sakeof readers.
REFERENCES:[1] H. Harada et al., Nuclear Data Sheets 118, p502
(2014).
[2] F.Kitatani et al., J. Nucl Sci. Tech. 51, p1107 (2014)[3] P. Schillebeeckx et al., Nuclear Data Sheets 113,
p3054 (2012).
[4] P. Schillebeeckx et al., JINST 7, C03009 (2012).

RESULTS: Figure 2 shows TOF neutron transmission
spectra. The ordinates are the normalized neutron counts,

採択課題番号 26044
中性子共鳴濃度分析法による溶融燃料等の核物質定量技術開発 通常採択
（原子力機構）北谷文人、土屋晴文、小泉光生、高峰潤（京大・原子炉）堀順一、佐野忠史、高橋佳之、中島健、宇根崎博信
147Test of a Microcell Multi-Wire Proportional Chamber for a Muon-Electron
Conversion Search Experiment, DeeMe

H. Natori, N. Abe1, M. Aoki2, Y. Igarashi, S. Ito2, S. Mihara, D. Nagao2, T. D. Nguyen2, T. M. Nguyen2, H.
Nishiguchi, Y. Seiya3, K. Shimizu3, T. Takahashi1,Y.
Takezaki3, N. Teshima3, K. Yamamoto3

after the blinded period. Because of the very high andrapid voltage up and down motion, readout electronics
suffers from large current input derived from the HV
switching. We also developed a readout system which
tolerates to high current input.

High Energy Accelerator Research Organization (KEK)
Research Reactor Institute, Kyoto University
2
Department of Physics, Osaka University
3
Department of Physics, Osaka City University

y[cm]

1

y[cm]

CO12-6

0.3

1400

0.3

1400

0.2

1200

0.2

1200

0.1

1000

0.1

1000

800

0

600

-0.1

INTRODUCTION: DeeMe [1] pursue mu-e conversion in nuclear field, which will be a clear evidence of the
new physics if it is found, because Standard Model of
elementary particle physics predicts it beyond an experimental reach. Detector is required to measure electron
momentum precisely after a huge pulse of prompt timing
charged particles, whose width and instantaneous hit rateis expected to be approximately 200ns and 70GHz/mm2.
Such a large input will make usual wire chamber detectors inactive due to space charge effect. We developed a
new technique to make a chamber to be tolerant to a large
input pulse.

Acrylic board& PMTsCherenkov light

1200

ADC

Accelerator

e- gunPulse electron Field emission electrons
200ns width
Flat time distribution
within 4us of RF injection

ND filter
Attenuate 10-3

0

0.14
x[cm]

0

600
400

-0.2
-0.3
-0.14

200
0

0.14
x[cm]

0

RESULTS: Fig. 3 shows an output result of the chamber. Electrons from beam gun tuned to be 70GHz/mm2 ininstantaneous hit rate are not amplified in the chamberwith applying pulsed high voltage to potential wire. This
enabled single electron detection coming after the burst
pulse. Noise derived from the HV switching is always thesame, so we can eliminate the noise by subtracting averaged waveform of plural numbers of events. We succeeded to obtain a clear electron signal after the burst
pulse avoiding the space charge effect by a burst pulse of
charged particles.
Noise by HV switching/work/deeme/data/kurri-201501//run02415.mid event number 121 channel 7

1000

MWPC

Accelerator

Collimator

200

-0.1

Fig. 2 Calculated electrical field contour. Anode-wire 1450V, Potential-wire 0V(left figure),
1450V(right figure)

EXPERIMENTS: Experimental setup is shown schematically in Fig. 1. Electron beam collimated to 16mm x
19mm penetrates Multi-Wire Proportional Chamber(MWPC) and beam counters. Beam rate is tuned changing current of electron gun heater.
Intensity control byheater power

400

-0.2
-0.3
-0.14

800

0

- A certain event- Average of many events- Subtracted waveform

800

Plastic
scintillator
& PMT

600

400

Singleelectron signal
200

Fig. 1 Schematics of experimental setup

0
52000

A huge pulse of prompt timing is emulated by tuned
pulse from electron beam gun. Delayed electron signals
are emulated by field emission electrons.
Electrical field contour inside the chamber calculated isshown in left of Fig. 2. Anode wires with 1450V and potential wires with 0V are put alternately. During a huge
pulse are coming, potential wires are applied with 1450V
as shown in right of Fig.2. With this setting, slope ofelectric field near anode wire become gentle that avalanche multiplication is suppressed. Temporary muting
the chamber during a burst pulse is expected to help tosuppress the space charge effect. Rectangular pulsed highvoltage is applied to potential wire to recover quickly

IHit^1

54000

56000

58000

60000

62000
time [ns]Fig. 3 Waveform of the chamber with electron
beam gun pulse and HV swithing

REFERENCES:[1] H. Natori, on behalf of the DeeMe Collaboration,
Nucl. Phys. B Proc. Suppl. Vol. 248-250 (2014)" r8jKlaJc:v
"hv

]R<5

"

通常採択

x  y3/;u&-BX#g0,$.Nx'6!.8[yqn=%wT)Mxp6!\ysPUW(fF7m     o>6Sx6pC6!\yZV9`Z_dY
bA*LG@eO?Q4E
148

CO12-7Ethnographic Study of Nuclear Reactor

M. Takagaki1,2, G. Shimazaki1, S. Masunaga3

self-righteously, once it fall into a little collapse,
lack of resilience of human wisdom for stabilization
and repair becomes embody.
By analyzing the narrative concerning the reactorof nuclear researchers, to describe the ethnographyof nuclear reactor and nuclear waste that is also a
study object of researchers themselves seems tolead to development of a new approach to themethodology of cultural anthropology. Such ethnography seems to be very useful for human society
by targeting to nuclear reactor as thing. Many nuclear physicists have focused on the following
statement of Prof. Wolfgang Weiss;

1

College of Nursing, Aino University
Graduate School of Human and Environmental Studies,
Department of Anthropology, Kyoto University
3
Graduate School of Science, Research Reactor Institute,
Kyoto University
2

Aside the pros and cons of the use of nuclear
power as an energy source, it seems to be useful inunderstanding the nuclear reactors to describe themas an ethnography based on the narrative data of
nuclear researchers. By describing the reactor as ascientific ethnography, it is expected to be highlighted the problem of nuclear reactors andlow-level radiation environment from a new angle.
Then, it is expected to provide further knowledge
for living in the contact zone between the field welive in safely (normal) and low-level radiation field(pathological), and going into patho and/or coexisting with patho.
This is a very unique study that an ethnographer
who is a radiation physicist, a physician and also ananthropologist participates in wide-range observation of nuclear research. The researchers have been
forced to include Fukushima as an enlarged research
field, and it is regarded as a chance to write up theexcellent scientific ethnography by doing this rather.
On 2014-2015, we have mainly investigated previous research, and preliminary investigation has been
carried out with biologists and physicists involvedin nuclear science at the Kyoto University. Theirnarrative indicated here was traumatic narrative of
Fukushima that suddenly appeared in their research
field of nuclear science. Sometime it was a narrativeof the confusion of the researchers themselves, although almost of the nuclear scientists have investigated sincerely with the nuclear reactor research as
an energy source of the human being. The radioactivity that has been discarded and released has been
completely isolated in a managed environment fromthe living space. Conversely, by this act, understanding of nuclear reactors and low-level radiation
environment, and also constructing networks among
various sub-specialists structurally become difficult.
The reason why researcher's confusion about Fukushima accident is so strong, I think because our
wisdom as the central pillar of our ego might be extremely imbalanced state. As being symbolicallyshown in Fukushima, because wisdom of nuclear
sciencehas
extremely
hypertrophied“The most serious damage caused by Fukushima
accident is that people lost trust for science andscientists. This certainly will influence long- term
human history, and we cannot recover such situation so easily. We scientists are responsible to suchsituation.”
Latour has pointed out that the dynamic and contingent elements intervene in the process of establishing the level of intellectual authority and knowledge
that circulates within the scientific community. Caseof Fukushima accident shows this extremely andplainly. It is expected to also lead to scientificachievements, such as actor network theory by scientific anthropological comparison analysis of thevarious disciplines of nuclear reactor researchers as
different cultures. And also, ethnographic researchmight be very helpful tool for well public understanding of reactor and/or low dose radiation field,
and then might regain confidence of scientists.
The understanding and knowledge of the researchers of KUR for their acceptance of this ambitious study is greatly appreciated. A new division
for Ethnographic Study for Nuclear Science is expected to be established in KUR. This research is
supported by Grant-in-Aid for Scientific Researchfor 2014-2016, No.26580152, JSPS. We are now
promoting our fieldwork and are planning to publish
ethnography of nuclear reactor on 2017.
REFERENCES:[1]K. Azuma, et al., Sekaishiso-sha. (2014)[2]B.Latour, Routeldge.(2013)[3]W.Allison, Wada Allison Pub. (2009)[4]AESJ, Fukushima Accident Report. Shinppyo-sha.
(2014)

	 採択課題番号26051
原子炉の人類誌	
 （藍野大学）高垣政雄、島崎義孝、（京大炉）増永慎一郎	
 
149

通常採択	
 

CO12-8

Effective Measures on Safety, Security, Hygiene and Disaster Preventionin Laboratories
USE & MANAGE OF SMALL AMOUNT of U & Th:
When using small amount of uranium or thorium up to
300g (DU, NU) and/or 900g (Th), most of safety control
procedures requested as radioactive materials are exempted by related regulations. Weighing control of nuclear elements is only requested by regulation. This
causes easy usage of uranium and thorium in laboratories.
For example, it is convenient that uranium acetate or uranium nitrate could be used for biology research to observe chromosomes clearly. Natural occurring radioactive
materials (NORM) such as minerals and seawater samples including uranium and thorium would also be troublesome sources which could be enriched through someresearch processes, and then would change into highconcentration radioactive materials as a result legally.
This is a representative technologically enhanced NORM(TENORM). TENORM is one of headache materials inlaboratory. Even the amount is quite small, the nuance ofterms of “nuclear” “uranium” and “thorium” will give a
big impact on society when some accidents or troubles
happen. We can use these materials easily and conveniently, however these are strictly controlled by the international regulations on their transfer. The latest guideline
on NORM and TENORM safety management by theJapanese regulatory body was published in 2009 to support the safety management. These situations must be
identified and understood by all stakeholders. Frameworkof related education for safety managers and users should
be adequately established and applied. All stakeholders
should understand their risk level and features of nuclear
materials as radioactive materials. This could lead reasonable and optimized safety management in laboratories.

T. Iimoto1, R. Hayashi1, T. Saito1, A. Yasmi1, S. Higaki1,
A. Sugiyama1, N. Kutsuna1, A. Kobashi1, K. Tanoi1, T.
Suzuki1, K. Kamiko1, T. Takahashi2, S. Takahashi2
1
2

The University of Tokyo
Research Reactor Institute, Kyoto University

INTRODUCTION:
Important research aspects can be found in the following
keywords such as safety, security, hygiene and disasterprevention. Nuclear research reactor is one of representative facilities together with these keywords under theiroperation. It is effective to investigate the latest status onpractical measures on these keywords in various facilities
including nuclear research reactors, to compare each other among facilities, and to discuss more effective or optimized ones for our positive safety management.
Through this process, it is also effective to investigate thelatest international and/or national regulations and the
movement of revision of them. This total discussion contents and its fruit 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.

NEXT RESEARCH TARGETS;
Education framework, curriculum and textbooks forsafety managers and users as well as relating officers tofill up the nuclear material controlling sheet for the use ofsmall amount of uranium and thorium should be discussed. This discussion should be based on the additional
investigation and analysis of the way to use, control andstorage the materials in laboratories.
REFERENCES:[1] T. IIMOTO, Environ. & Safety, 4(3),1-8 (2013)

Discussion target in BY of 2014 was determined as“safety control in use of small amount nuclear materials”
through our internal member discussion. We investigated
the related regulations and their application as well as thefact-finding in use of small amount of uranium and thorium in Japanese laboratories.

[2]T. IIMOTO et.al., Safety Engineering,48(4),215-221(2009)[3] T.IIMOTO et.al., Isotope News, 566,64-67, (2001)[4] MEXT, Guideline for Safety Management of NORM
and Consumer Products (2009)

採択課題番号 26054

実験施設における安全衛生・セキュリティ・防災等の通常採択
効果的な対応と対策に関する研究(東大)飯本武志、林瑠美子、齊藤拓巳、安見厚志、桧垣正吾、杉山 暁、朽名夏麿、小橋浅哉、
田野井慶太郎、鈴木崇彦、神子公男、布川 淳、小原佑介、前寺郁彦（京大・原子炉）高橋知之、
高橋千太郎

150

CO12-9Development of New NiMo Neutron Mirror for Fundamental Physics

Y. Arimoto1, P. Geltenbort2, S. Imajo3, Y. Iwashita4,
M. Hino5, R. Katayama6, M. Kitaguchi7, K. Mishima1, R.
Sakakibara7, Y. Seki8, H. M. Shimizu7 and T. Yoshioka9

The facts of (1) and (2) help us to understand what phenomenon occurred while NiMo ingot evaporating. These
are as follows:1

KEK,2ILL, 3Dep. of Phys. Kyoto Univ.,4ICR Kyoto Univ.,
KURRI, 6Dep. of Phys. Univ. of Tokyo, 7Dep. of Phys.
Nagoya Univ., 8Sch. of Eng. Univ. of Tokyo, 9Dep. of Phys.
Kyushu Univ.
5(a) There is a possibility that NiMo ingot material included gasses and it caused bumping phenomenon of(2). If it true, gasses could also affect the density decrease of (1).
(b) The deposited NiMo films preserve the nature of NiMo alloy; Otherwise, the density of test samples
should close to the one expected for Ni, 8.9 g/cm3,
because the Ni vapor pressure is 105 times higher than
Mo at 2000 K.
(c) In spite of (b), the vapor pressure of NiMo alloy wasquite low. Probably, NiMo vapor was not efficiently
transported at substrates from evaporation source position, which could cause the density decrease of (1).
(d) There is a possibility that the crystal structure of thedeposited NiMo films varied from that of NiMo ingot.
If it true, it could affect the density decrease of (1).

INTRODUCTION: A large amount of CP violation(CPV) is necessary to solve matter and anti-matterasymmetry problem in the universe. However, theamount of CPV standard model predicts is too insufficient to explain it. The fact indicates that the new physics
beyond standard model (BSM) exists and supplies thelack of CPV. The neutron intrinsic electric dipole moment(nEDM) is sensitive to CPV that BSM provides. Therefore, we can effectively search BSM with precise nEDM
measurement.
The nEDM can be obtained from the ultracold neutron(UCN) spin precession in a storage container under homogeneous electric and magnetic fields. In the experiment, the loss of UCNs and their polarization occur due
to interaction between UCNs and wall material, whichmake statistical precision worse. It is therefore important
to develop new wall material with low loss probabilities.
On the other hand, in the case that UCNs are transported
from a pulsed UCN source, by decelerating fast UCNs
and/or by accelerating slow UCNs properly, these UCNs
can be focused on a storage container at the same time,
which achieves drastic improvement of statistical precision [1]. However, if diffuse scattering induced by roughwall arises, the degree of improvement decreases. It is
hence also important to develop a wall material with assmooth surfaces as neutron mirrors have.

(a), (b), (c) and (d) give us quite an important information
for next desirable fabrication test with vacuum evaporation deposition. First, we should use degassed NiMo ingot to solve the problem of (a). Second, to compensate
the shortage of NiMo vapor pressure ((b) and (c)), a next
vacuum evaporated deposition should be conducted byattracting ionized NiMo vapor to substrates with a bias
voltage. Third, to avoid structure change of (d), Ni andMo are evaporated simultaneously so that the composition of deposited NiMo film becomes 15 weight percent
and 9.1 g/cm3.
SUMMARY: The material with low loss probabilities
and smooth surfaces is desired for nEDM experiment.
NiMo of 15 weight percent and 9.1 g/cm3 is known as
one of the promising low loss materials. We therefore
fabricated test samples using NiMo ingot with KURRI
vacuum evaporated apparatus. Although we succeeded in
NiMo film deposition itself, the densities of test samples
were only 6.3 to 6.6 g/cm3, and these surfaces were toorough to use neutron mirrors. To solve these problems, it
is desirable that next fabrication with vacuum evaporation deposition should be performed using two evaporation source of degassed Ni and Mo ingot, and by attracting ionized NiMo vapor to substrates with a bias voltage.

Ni-Mo FABRICATION WITH VACUUM EVAPORATED MACHINE: Nickel-Molibdenum alloy (NiMo)
of 15 weight percent and 9.1 g/cm3 is known as one ofthe promising low loss materials. We fabricated test samples made of NiMo with KURRI vacuum evaporated
apparatus and aimed for 100 nm thickness on SUS304
and Si-wafer substrates.
RESULT AND CONSIDEREATION: We succeeded in
NiMo film deposition itself. However, two undesirable
features appeared as follows:

REFERENCES:[1] Y. Arimoto et al., Phys. Rev. A86 (2012) 023843.

(1) The densities of test samples were only 6.3 to 6.6
g/cm3 by measuring XRR, which is far less than expected value, 9.1 g/cm3. Hence, our deposited NiMo
film cannot be used as a wall material for nEDM.
(2) In this fabrication, a bumping phenomenon could not
be suppressed. Consequently, these surfaces were sorough that it could not be used as neutron mirrors.

採択課題番号 26059 題名白色ビーム対応多層膜中性子干渉計のためのスーパーミラーの開発 II（東大院・工）関義親（名大院・理）北口雅暁（京大原子炉）日野正裕

151

通常採択

II. PUBLICATION LIST(APRIL 2014 – MARCH 2015)152

1. Slow Neutron Physics and Neutron Scattering
PapersDistinct Features of the Histone Core Structure in Nucleosomes Containing the Histone H2A.B Variant
M. Sugiyama, Y. Arimura, K. Shirayama, R. Fujita, Y. Oba, N. Sato, R. Inoue, T. Oda, M. Sato, R. K. Heenan and
H. Kurumizaka
Biophysical Journal, 106 (2014) 2206-2213.
A Novel Magnet Design Using Coated Conductor for Spiral Sector FFAG Accelerators
K. Goda, N. Amemiya, T. Nakamura, Y. Mori, T. Ogitsu, T. Kurusu and M. Yoshimoto
IEEE TRANSACTIONS ON APPLIED SUPERCONDUCTIVITY, 24 (2014) 4402605.
Conformational Characterization of a Protein Complex Involving Intrinsically Disordered Protein by Small-angle
Neutron Scattering Using the Inverse Contrast Matching Method: a Case Study of Interaction Between α-synuclein
and PbaB Tetramer as a Model Chaperone
M. Sugiyama, H. Yagi, T. Yamaguchi, K. Kumoi, M. Hirai, Y. Oba, N. Sato, L. Porcar, A. Martel and K. Kato
J. Appl. Crystallogr., 47 (2014) 430-435.
Development of Highly-mechanically Polished Metal-substrate for Neutron Supermirrors
S. Takeda, J. Guo, S. Morita, H. Ono, T. Oda, J. Kato, H. Sato, M. Hino, Y. Yamagata and M. Furusaka
J. Phys. Conf. Ser., 528 (2014) 12011-6.
Production of Ultra cold Neutrons by a Doppler Shifter with Pulsed Neutrons at J-PARC
K. Mishima, S. Imajo, M. Hino, T. Ino, Y. Iwashita, R. Katayama, M. Kitaguchi, T. Oda, H. M. Shimizu, M. Utsuro,
S. Yamashita and T.Yoshioka
J. Phys. Conf. Ser., 528 (2014) 12030-8.
Temperature Dependence of the Nanostructure in a PbSe–ZnSe Composite thin Film
Y. Oba, S. Abe, M. Ohnuma, N. Sato and M. Sugiyama
J. Phys. D: Appl. Phys., 47 (2014) 6.
New Fabrication Method for an Ellipsoidal Neutron Focusing Mirror with a Metal Substrate
J. Guo, S. Takeda, S. Morita, M. Hino, T. Oda, J. Kato, Y. Yamagata and M. Furusaka
Opt. Express., 22 (2014) 24666-24677.
Observation of the Spatial Distribution of Gravitationally Bound Quantum States of Ultracold Neutrons and Its
Derivation Using the Wigner Function
G. Ichikawa, S. Komamiya, Y. Kamiya, Y. Minami, M. Tani, P. Geltenbort, K. Yamamura, M. Nagano, T. Sanuki,
S. Kawasaki and M. Hino
Phys. Rev. Lett., 112 (2014) 71101.
Distribution of Glass Transition Temperature in Multilayered Poly (Methyl Methacrylate) Thin Film Supported on a
Si Substrate as Studied by Neutron Reflectivity
R. Inoue, M. Nakamura, K. Matsui, T. Kanaya, K. Nishida and M. Hino
Phys. Rev. E, 88 (2014) 32601.
Numerical Simulation of BL06 Neutron Beamline for "VIN ROSE" at J-PARC/MLF
T. Oda, M. Hino, M. Kitaguchi, Y. Kawabata, N. L. Yamada and H. Seto
Progress in Nuclear Science and Technology, 4 (2014) 214-217.

153

Structure of Silver Bromide Doped Chalco Genide Glasses
Y. Onodera, T. Usuki, T. Nasu and S. Kohara
Solid State Ionics, 262 (2014) 469-471.
Books
Hemoglobin (Crystallography in Japan (II)) (in Japanese)
Y. Morimoto
Crystallographic Society of Japan, (2014).
Reviews
Structural Study of Amorphous and Nano-crystalline Materials by Neutron Scattering (in Japanese)
T. Fukunaga
HAMON, 24 (2014) 94-99.
2. Nuclear Physics and Nuclear Data
PapersThe Influence of p53 Status in Glioblastoma on the Effects of Boron Neutron Capture Therapy
K. Seki, Y. Kinashi and S. Takahashi
Anticancer Res., 35 (2015) 169-174.
A Nuclear Data Project on Neutron Capture Cross Sections of Long-Lived Fission Products and Minor Actinides
M. Igashira, T. Katabuchi, H. Harada, S. Nakamura, A. Kimura, N. Iwamoto, J. Hori and Y. kiyanagi
Nucl. Data Sheets, 118 (2014) 72-77.
Cross Section Measurement of 237Np(n, g) at J-PARC/MLF/ANNRI
K. Hirose, K. Furutaka, K. Y. Hara, H. Harada, J. Hori, M. Igashira, T. Kamiyama, T. Katabuchi, A. Kimura, T. Kin,
F. Kitatani, Y. Kiyanagi, M. Koizumi, M. Mizumoto, S. Nakamura, M. Oshima and Y. Toh
Nucl. Data Sheets, 119 (2014) 48-51.
Capture Gross-section Measurement of 241Am(n, g) at J-PARC/MLF/ANNRI
H. Harada, M. Ohta, A. Kimura, K. Furutaka, K. Hirose, K. Y. Hara, T. Kin, F. Kitatani, M. Koizumi, S. Nakamura,
M. Oshima, Y. Toh, M. Igashira, T. Katabuchi, M. Mizumoto, K. Kino, Y. Kiyanagi, T. Fujii, S. Fukutani, J. Hori
and K. Takamiya
Nucl. Data Sheets, 119 (2014) 61-64.
Measurements of Capture Gamma Rays from the Neutron Resonances of 74Se and 77Se at J-PARC/MLF/ANNRI
J. Hori, H. Yashima, S. Nakamura, K. Furutaka, K. Y. Hara, H. Harada, K. Hirose, A. Kimura, F. Kitatani, M.
Koizumi, M. Oshima, Y. Toh, M. Igashira, T. Katabuchi, M. Mizumoto, T. Kamiyama, K. Kino and Y. Kiyanagi
Nucl. Data Sheets, 119 (2014) 128-131.
Measurement of Capture Gamma Rays from 99Tc Neutron Resonances at the J-PARC/ANNRIK. Kino, F. Hiraga, T. Kamiyama, Y. Kiyanagi, H. Harada, K. Y. Hara, K. Hirose, A. Kimura, F. Kitatani,
S. Nakamura, M. Igashira, T. Katabuchi, M. Mizumoto and J. Hori
Nucl. Data Sheets, 119 (2014) 140-142.
Cross Section Measurements of the Radioactive 107Pd and Stable 105, 108Pd Nuclei at J-PARC/MLF/ANNRI
S. Nakamura, A. Kimura, F. Kitatani, M. Ohta, K. Furutaka, S. Goko, K. Y. Hara, H. Harada, K. Hirose, T. Kin, M.
Koizumi, M. Oshima, Y. Toh, K. Kino, F. Hiraga, T. Kamiyama, Y. Kiyanagi, T. Katabuchi, M. Mizumoto,M. Igashira, J. Hori, T. Fujii, S. Fukutani and K. Takamiya
Nucl. Data Sheets, 119 (2014) 143-146.

154

Measurements of Neutron Capture Cross Sections of 112Sn and 118Sn with J-PARC/MLF/ANNRI
A. Kimura, K. Hirose, S. Nakamura, H. Harada, K. Y. Hara, J. Hori, M. Igashira, T. Kamiyama, T. Katabuchi,
K. Kino, F. Kitatani, Y. Kiyanagi, M. Koizumi, M. Mizumoto and Y. Toh
Nucl. Data Sheets, 119 (2014) 150-153.
Measurements of Cross Sections for Neutron-induced Reactions on Chromium and Yttrium Targets at 197 MeV
S. Sekimoto
Nucl. Data Sheets, 119 (2014) 197-200.
A New Signal Processing Technique for Neutron Capture Cross Section Measurement Based on Pulse Width
Analysis
T. Katabuchi, T. Matsuhashi, K. Terada, M. mizumoto, K. Hirose, A. Kimura, K. Furutaka, K. Y. Hara, H. Harada,
J. Hori, M. igashira, T. Kamiyama, F. Kitatani, K. Kino, Y. Kiyanagi, M. Koizumi, S. Nakamura, M. Oshima andY. TohNucl. Data Sheets, 119 (2014) 398-400.
Measurements of High-Energy Excited States and γ-Rays of Fission Products with a 4π Clover Detector
Y. Shima, Y. Kojima, H. Hayashi, A. Taniguchi and M. Shibata
Nucl. Data Sheets, 120 (2014) 30-32.
Half-Life Measurements of Excited Levels in Fission Products around Mass Number 150
Y. Kojima, Y. Shima, H. Hayashi, A. Taniguchi and M. Shibata
Nucl. Data Sheets, 120 (2014) 52-55.
Energy Resolution of Pulsed Neutron Beam Provided by the ANNRI Beamline at the J-PARC/MLF
K. Kino, M. Furusaka, F. Hiraga, T. Kamiyama, Y. Kiyanagi, K. furutaka, S. Goko, K. Y. Hara, H. Harada, M.
Harada, K. Hirose, M. Ooi, M. Ohta, M. Oshima, Y. toh, M. Igashira, T. Katabuchi, M. Mizumoto and J. Hori
Nucl. Instrum. Methods, A 736 (2014) 66-74.
Pulse-width Analysis for Neutron Capture Cross-section Measurement Using an NaI(Tl) Detector
T. Katabuchi, T. Matsuhashi, K. Terada, T. Arai, K. Furutaka, K. Y. Hara, H. Harada, K. Hirose, J. Hori, M. Igashira,T. Kamiyama, A. Kimura, K. Kino, F. Kitatani, Y. Kiyaangi, M. Koizumi, M. Mizumoto, S. Nakamura, M. Oshima
and Y. Toh
Nucl. Instrum. Methods. Phys. Res. A, 764 (2014) 369-377.
Radiation Shielding Experiments for Composites Based on Pb-shot and Boride
J. Hori, H. Yashima, K. Miyamoto, S. Okuda, M. Ishihara, S. Kito and M. Atarashi
Progress in Nuclear Science and Technology, 4 (2014) 635-638.
Measurements of the Neutron Activation Cross Sections for Bi and Coat 386 MeV
H. Yashima, S. Sekimoto, K. Ninomiya, Y. Kasamatsu, T. Shima, N. Takahashi, A. Shinohara, H. Matsumura,
D. Satoh, Y. Iwamoto, M. Hagiwara, K. Nishiizumi, M.W. Caffee and S. Shibata
Radiat. Prot. Dosimetry, 161 No. 1-4 (2014) 139-143.
New Application for Boron Neutron Capture Therapy
M. Suzuki
Radioisotopes, 64 (2015) 59-66.
Proceedings
Measurement of Neutron Capture Cross Section of 232TH in the Low Energy Region
J. Hori, T. Sano, Y. Takahashi, H. Unesaki and K. Nakajima
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014) 1.

155

Survey on Effect of Crystal Texture of Beryllium on Total Cross-Section to Improve Neutronic Evaluation in JMTR
N. Takemoto, T. Imaizumi, N. Kimura, K. Tsuchiya, J. Hori, T. Sano and K. Nakajima
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014) 1.
Development of a New Type of Manganese Bath for Determination of Neutron Emission Rate of a Neutron Source
T. Matsumoto, H. Harano, A. Masuda and J. Hori
2014 IEEE Nuclear Science Symposium, Seattle, USA (Nov. 8-15, 2014) 1-5.
Development of a Neutron Transport System for Neutron Resonance Densitometry
F. Kitatani, M. Koizumi, H. Tsuchiya, J. Takamine, M. Kureta, H. Harada, M. Seya, J. Hori and T. Sano
Proc. of the 49th KURRI Scientific Meeting, KURRI (Jan. 28-29, 2015) 41.
Reviews
Kyoto University Research Reactor Institute Electron Linear Accelerator Neutron Source (in Japanese)
J. Hori, T. Sano and Y. Takahashi
Isotope News, 717 (2014) 38-40.
3. Reactor Physics and Reactor Engineering
PapersA New Concept of Monte Carlo Kinetics Parameter Calculation Using Complex-valued Perturbation
T. Yamamoto and H. Sakamoto
Ann. Nucl. Energy., 71 (2014) 480-488.
Optimised Mounting Conditions for Poly (Ether Sulfone) in Radiation Detection
H. Nakamura, Y. Shirakawa, N. Sato, T. Yamada, H. Kitamura and S. Takahashi
Int. J. Rad. Appl. Instrum. A, 91 (2014) 131.
Measurements of Turbulence in a Liquid-metal Two-phase Flow by Using Miniture Electro-magnetic Probe
G. Ariyoshi, Y. Asai, D. Ito, Y. saito and K. Mishima
Japanease Journal of Multiphase Flow, 27-5 (2014) 615-622. (in Japanese)
Heat Transfer Study for ADS Solid Target - Surface Wettability and its Effect on a Boiling Heat TransferD. Ito, K. Hase and Y. Saito
Nuclear Backend and Transmutation Technology for Waste Disposal: Beyond the Fukushima Accident,
ISBN 978-4-431-55110-2 (2014) 95-105.
Experimental Study of Flow Structure and Turbulent Characteristics in Lead-bismuth Two-phase Flow
G. Ariyoshi, D. Ito and Y. Saito
Nuclear Backend and Transmutation Technology for Waste Disposal: Beyond the Fukushima Accident,
ISBN 978-4-431-55110-2 (2014) 107-115.
HeteroGeneity Effect on Neutron Shielding in Borated Concrete and Monte Carlo-Based Cross Section
Homogenization Method for Particle Dispersed MediaT. Yamamoto
Progress in Nuclear Science and Technology, 4 (2014) 404-407.
Undoped Poly (Phenyl Sulfone) for Radiation Detection
H. Nakamura, Y. Shirakawa, N. Sato, H. Kitamura and S. Takahashi
Radiat. Meas., 73 (2015) 14.

156

Implications for Quinone Cofactor Biogenesis in Amine-oxidizing Enzymes
A. Kita, M. Mure and K. Miki
SPring-8/SACLA Research Report, SectionA, Vol.3, No. 1 (2015) 1-5.
Proceedings
Implementation of Two-group Interfacial Area Transport in a One-dimensional Computational Environment
J.P. Schlegel, T. Hibiki, M. Ishii, X. Shen and S. Appathurai
Proceeding of International Topical Meeting on Advances in Thermal Hydraulics 2014 (ATH'14)
Reno, Nevada, USA, Paper No.: 042 (Jun. 15-19, 2014) 555-567.
Experimental Benchmarks on the Thorium-Loaded Accelerator-Driven System at the Kyoto University Critical
Assembly
C. H. Pyeon
Technical Mtg. (TM) of “Collaborative Work on Accelerator Driven Subcritical Systems (ADS) and Use of LowEnriched Uranium (LEU) in ADS” (invited), IAEA, Hefei, China (Sept. 8-12, 2014).
Preparation of Minor Actinides Irradiation in Accelerator-Driven System with 100 MeV Protons at Kyoto University
Critical Assembly
T. Yagi, C. H. Pyeon, Y. Takahashi and K. Nakajima
Proc. Actinide and Fission Product Partitioning and Transmutation, Thirteenth Information and Exchange Mtg(13IEMPT), OECD/NEA, Seoul, Korea (Sept. 23-26, 2014).
Investigation on Subcriticality Measurement Using Inherent Neutron Source in Nuclear Fuel
T. Shiozawa, T. Endo, A. Yamamoto, C.H. Pyeon and T. Yagi
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).
Concept of Capture Credit Based on Neutron Induced Gamma Ray Spectroscopy
Y. Nauchi, H. Ohta, H. Unesaki, T. Sano and T. Yagi
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014) 1.
Neutronic Characteristics of Solid Pb-Bi Target in Accelerator-Driven System at Kyoto University Critical Assembly
C. H. Pyeon, H. Nakano, M. Yamanaka, T. Yagi and T. Misawa
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).
Monte Carlo Perturbation Analysis on Isothermal Temperature Reactivity Coefficient of Light-Water Moderated andReflected Critical Assembly
B. K. Jeon, H. J. Shim and C. H. Pyeon
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).
Measurement of Subcriticality Using Delayed Neutron Source Combined with Pulsed Neutron Accelerator
T. Misawa, T. Yagi, and C. H. Pyeon
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).
Measurement of Large Negative Reactivity of an Accelerator-Driven System in the Kyoto University Critical
Assembly
A. Sakon, K. Hashimoto, M. A. Maarof, M. Kawasaki, W. Sugiyama, C. H. Pyeon, T. Sano, T. Yagi and T. Ohsawa
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).
Accuracy of Thorium-Loaded Accelerator-Driven System at Kyoto University Critical Assembly
M. Yamanaka, C. H. Pyeon, T. Yagi and T. Misawa
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).

157

Analysis of Integral Experiment for Thorium Fuel Cycle at Kyoto University Critical Assembly
Y. Takahashi, T. Sano, J. Hori, H. Unesaki and K. Nakajima
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct. 3, 2014).
Void Transit Time Calculations by Neutron Noise of Propagation Perturbation Using Complex-valued
Weight Monte CarloT. Yamamoto
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct.3, 2014).
Power Spectral Analysis for a Subcritical Reactor System Driven by a Pulsed Spallation Neutron Source
A. Sakon, S. Hohara, W. Sugiyama, K. Hashimoto, C. H. Pyeon, T. Sano and T. Yagi
PHYSOR2014, Kyoto, Japan (Sept. 28- Oct.3, 2014) 1.
Statistical Error Estimation Using Bootstrap Method for the Feynman-α method
T. Endo, T. Shiozawa, A. Yamamoto, C.H. Pyeon and T. Yagi
ANS 2014 Winter Meeting, Anaheim, CA, USA (Nov. 9-13, 2014) 1204-1207.
Study on Boiling Heat Transfer for ADS Solid Target - Surface Wettability & Micro-Bubble Emission Boiling D. Ito, M. Kato and Y. Saito
9th Korea-Japan Symposium on Nuclear Thermal Hydraulics and Safety (NTHAS-9),
Buyeo, Korea (Nov. 16-19, 2014) 49.
Local Measurements of 3-D Bubble Velocity Vector, Bubble Diameter and Interfacial Area Concentration in a
Vertical Large Diameter Square Duct
X. Shen, T. Hibiki, H. Sun and H. Nakamura
Proceeding of the 9th Japan-Korea Symposium on Nuclear Thermal Hydraulics and Safety (NTHAS-9),
Buyeo, Korea (Nov. 16-19, 2014) N9P0011.
Books
Frontiers and Progress in Multiphase Flow I (in Japanese)(Chapter 2 Flow Characteristics and Void Fraction Prediction in Large Diameter Pipes)
X. Shen, JP Schlegel, P. Joshua, S. Chen, S. Rassame, MJ. GriffithsMatthew, T. Hikiki and M. Ishii
Springer, (2014).
OthersIncrement of Capacity of Casks for LWR Spent Fuel Transport (3) DemonStration of Quantification of Neutron
Leakage from a Fuel Assembly
Y. Nauchi, T. Kameyama, H. Unesaki, T. Misawa, T. Sano and T. Yagi
CRIEPI Research Report, L11004 (2012).
4. Material Science and Radiation Effects
PapersThe Spin State of Iron in Fe3+-bearing Mg-perovskite and Its Crystal Chemistry at High Pressure
I. Mashino, E. Ohtani, N. Hirao, T. Mitsui, R. Masuda, M. Seto, T. Sakai, S. Takahashi and S. Nakano
Am. Mineral., 99 (2014) 1555-1561.
Frequency Domain Monte Carlo Simulation Method for Cross Power Spectral Density Driven by Periodically Pulsed
Spallation Neutron Source Using Complex-valued Weight Monte CarloT. Yamamoto
Ann. Nucl. Energy., 63 (2014) 711-720.

158

A Neutron Dynamic Therapy with a Boron Tracedrug UTX-51 Using a Compact Neutron Generator
H. Hori, R. Tada, Y. Uto, E. Nakata, T. Morii and K. Masuda
Anticancer Res., 34 (2014) 4557-4560.
Positron Annihilation Study for Enhanced Nitrogen-vacancy Center Formation in Diamond by Electron Irradiation
at 77K
Z. Tang, T. Chiba, Y. Nagai, K. Inoue, T. Toyama and M. Hasegawa
Appl. Phys. Lett., 104 (2014) 72101.
Synchrotron Radiation-Based Mössbauer Spectra of 174Yb Measured with Internal Conversion Electrons
R. Masuda, Y. Kobayashi, S. Kitao, M. Kurokuzu, M. Saito, Y. Yoda, T. Mitsui, F. Iga and M. Seto
Appl. Phys. Lett., 104 (2014) 82411.
Dose-rate Effect was Obsereved in T98G Glioma Cells Following BNCT
Y. Kinashi, K. Okumura, Y. Kubota, E. Kitajima, R. Okayasu, K. Ono and S. Takahashi
Appl. Radiat. Isot., 88 (2014) 81-85.
Facile One-Pot Synthesis of [1, 2, 3]Triazolo[1, 5-a]Pyridines from 2-Acylpyridines by Copper(II)-Catalyzed
Oxidative N-N Bond Formation
T. Hirayama, S. Ueda, T. Okada, N. Tsurue, K. Okuda and H. Nagasawa
Chem. Eur. J., 20 (2014) 4156.
Extranuclear Dynamics of 111Ag(→111Cd) Doped in AgI Nanoparticles
W. Sato, R. Mizuuchi, N. Irioka, S. Komatsuda, S. Kawata, A. Taoka and Y. Ohkubo
Chem. Phys. Lett., 609 (2014) 104-107.
Predominance of Covalency in Water-Vapor-Responsive MMX-Type Chain Complexes Revealed by 129I Mössbauer
Spectroscopy
H. Iguchi, S. Kitao, M. Seto, S. Takaishi and M. Yamashita
Dalton Trans., 43 (2014) 8767-8773.
Slow Dynamics of Supercooled Liquid Revealed by Rayleigh Scattering of M&oumlssbauer Radiation Method inTime Domain
M. Saito, A. Battistoni, S. Kitao, Y. Kobayashi, M. Kurokuzu, Y. Yoda and M. Seto
Hyperfine Interact., 226 (2014) 629-636.
Development of 125Te Synchrotron-Radiation-Based M&oumlssbauer Spectroscopy
M. Kurokuzu, S. Kitao, Y. Kobayashi, M. Saito, R. Masuda, T. Mitsui, Y. Yoda and M. Seto
Hyperfine. Interact, 226 (2014) 687-691.
Boron Neutron Capture Therapy for Advanced Salivary Gland Carcinoma in Head and Neck
T. Aihara, N. Morita, N. Kamitani, H. Kumada, K. Ono, J. Hiratsuka and T. HaradaInt. J. Clin. Oncol., 19 (2014) 437-444.
Effects of Mg Substitution on Crystal Structure and Hydrogenation Properties of Pr 1–xMgxNi3
K. Iwase, N. Terashita, K. Mori, S. Tashiro, H. Yokota and T. Suzuki
Int. J. Hydrogen Energy, 39 (2014) 12773-12777.
Formation Energy of Oxygen Vacancies in ZnO Determined by Investigating Thermal Behavior of Al and In
Impurities
S. Komatsuda, W. Sato and Y. Ohkubo
J. Appl. Phys., 116 (2014) 183502.

159

Relaxation Transition in Glass-forming Polybutadiene as Revealed by Nuclear Resonance X-ray Scattering
T. Kanaya, R. Inoue, M. Saito, M. Seto and Y. Yoda
J. Chem. Phys., 140 (2014) 144906.
Spatial Correlation between Chemical and Topological Defects in Vitreous Silica: Uvresonance Raman Study
M. Saito, F. D’Amico, F. Bencivenga, R. Cucini, A. Gessini, E. Principi and C. Masciovecchio
J. Chem. Phys., 140 (2014) 244505.
Selective Hg(II) Adsorption from Aqueous Solutions of Hg(II) and Pb(II) by Hydrolyzed Acrylamide-grafted PET
Films
N. Rahman, N. Sato, M. Sugiyama, Y. Hidaka, H. Okabe and K. Hara
J. Environ. Sci. Health. A, 49 (2014) 798-806.
Early Stage Irradiation Effects in F82H Model Alloys
S.S. Huang, X.Q. Pan, K. Sato, Q. Xu and T. Yoshiie
J. Nucl. Mater., 449 (2014) 248-251.
A replica Technique for Extracting Precipitates from Neutron-irradiated or Thermal-aged Vanadium Alloys for TEM
Analysis
K. Fukumoto and M. Iwasaki
J. Nucl. Mater., 449 (2014) 315-319.
Studies on ADS as a neutron source at the Kyoto University Research Reactor Institute
T. Yoshiie, K. Fukumoto, Y. Ishi, D. Ito, Y. Kuriyama, T. Misawa, Y. Mori, T. Nagasaka, K. Nakajima, Y. Oki,
C.H. Pyeon, Y. Saito, K. Sato, X.Z. Shen, S. Shibata, T. Uesugi and Q. Xu
J. Nucl. Mater., 450 (2014) 16-19.
Positron Annihilation Spectroscopy of Ferritic/Martensitic Steels F82H and T91 Irradiated with Protons and Neutrons
at PSI
K. Sato, S. Kawamoto, K. Ikemura, V. Krsjak, C. Vieh, R. Brun, Q. Xu, T. Yoshiie and Y. Dai
J. Nucl. Mater., 450 (2014) 59-63.
Positron Annihilation and TEM Studies in Ion Irradiated Fe and Fe-Cr Model Alloys of Ferritic/Martensitic SteelQ. Xu, Y. Sugiura, X.Q. Oan, K. Sato, T. Yoshiie, H. Tsuchida and A. ItohJ. Nucl. Mater., 455 (2014) 122-125.
Structural Origin of Ionic Conductivity for Li7P3S11 Metastable Crystal by Neutron and X-ray Diffrcation
Y. Onodera, K. Mori, T. Otomo, H. Arai, Y. Uchimoto, Z. Ogumi and T. Fukunaga
J. Phys. Conf. Ser., 502 (2014) 12021.
Formation of Cu Precipitates in A High-Energy-Particle-Irradiated and Thermally Aged Fe-0.6Cu Alloy
K. Sato, Q. Xu, X.Z. Cao, P. Zhang, B.Y. Wang and H. Tsuchida
J. Phys. Conf. Ser., 505 (2014) 12011.
Positron Beam Facility at Kyoto University Research Reactor
Q. Xu, K. Sato, T. Yoshiie, T. Sano, H. Kawabe, Y. Nagai, K. Nagumo, K. Inoue, T. Toyama, N. Oshima,
A. Kinomura and Y. Shirai
J. Phys. Conf. Ser., 505 (2014) 12030.
Thermal Stability of Locally-Associated Al and In Impurities in Zinc Oxide
S. Komatsuda, W. Sato and Y. Ohkubo
J. Radioanal. Nucl. Chem., (2014) 1249-1252.

160

Hierarchical Structure−property Relationships in Graft-type Fluorinated Polymer Electrolyte Membranes Using
Small- and Ultrasmall-angle X-ray Scattering Analysis
T. D. Tap, S. Sawada, S. Hasegawa, K. Yoshimura, Y. Oba, M. Ohnuma, Y. Katsumura and Y. Maekawa
Macromolecules, 47 (2014) 2373-2383.
Comparison between In-Situ and Post-Irradiation Cyclic Deformation Structures in Ni by 150 MeV Proton Irradiation
T. Yoshiie, K. Sato, Q. Xu, Y. Ishi, T. Uesugi, Y. Kuriyama and Y. Mori
Mater. Trans., 55 (2014) 434-437.
Surface Observation of LaNi5 under Deuterium Atmosphere Using Small-Angle Neutron Scattering
K. Mori, K. Iwase, Y. Oba, T. Fukunaga and M. Sugiyama
Mater. Trans., 55 (2014) 1643-1646.
High-pressure Radiative Conductivity of Dense Silicate Glasses with Potential Implications for Dark-magmas
M. Murakami, A. F. Goncharov, N. Hirao, R. Masuda, T. Mitsui, S-M. Thomas and C. R. Bina
Nat. Commun., 5 (2014) 5428.
Positron Annihilation Study of Vacancy-Type Defects in Fast-Neutron-Irradiated MgO/nAl2O3
A.Z.M.S. Rahman, Z.X. Li, X.Z. Cao, B.Y. Wang, L. Wei, Q. Xu and K. Atobe
Nucl. Instr. & Meth. Pyhs. Res. B, 335 (2014) 70-73.
Neutron-enhanced Annealing of Ion-implantation Induced Damage in Silicon Heated by Nuclear Reactions
A. Kinomura, T. Yoshiie, A. Chayahara, Y. Mokuno, N. Tsubouchi, Y. Horino, Q. Xu, K. Sato, K. Yasuda and
R. Ishigami
Nucl. Instrum. Methods. Phys. Res. B, 334 (2014) 48-51.
Material Activation Benchmark Experiments at the NuMI Hadron Absorber Hall in Fermilab
H. Matsumura, N. Matsuda, Y. Kasugai, A. Toyoda, H. Yashima, S. Sekimoto, H, Iwase, K. Oishi, Y. Sakamoto,
H. Nakashima, A. Leveling, D. Boehnlein, G. Lauten, N. Mokhov and K. Vaziri
Nuclear Data Sheets, 120 (2014) 219-221.
Hydrogen Trapping under the Effect of W-C Mixed Layers
N. Liu, J. Huang, K. Sato, Q. Xu, L. Q. Shi and X. Y. Wang
Nucl. Fusion, 54 (2014) 33013.
Determination of Dynamical Parameters in Liquids by Homodyne Transient Grating Spectroscopy at Large Angles
R. Cucini, A. Battistoni, A. Gessini, F. Bencivenga, E. Principi, M. Saito, F. D'Amico, R. Sergo and C. Masciovecchio
Optics Letters, 39 (2014) 5110-5113.
Detection of Boron-Containing Amino Acids and Peptides Using Fluorescent Boron-Sensor
Y. Hattori, M. Ishimura, Y. Ohta, H. Takenaka and M. Kirihata
Peptide Science 2014, (2014) 295.
Studies of Interaction between He and Elements with Mass Number 140 in Fe by Time-Differential PerturbedAngular-Correlation Measurements
Y. Ohkubo, A. Taniguchi, Q. Xu, M. Tanigaki and K. Sato
Philos. Mag. Lett., 94 (2014) 470-477.
Neutron-irradiation-induced Near-infrared Emission in Alpha-Al2O3
A. Z. M. S. Rahman, X. Cao, L. Wei, B. Wang, H. Ji, T. Yang, Q. Xu and K. Atobe
Philos. Mag. Lett., 94 (2014) 211-216.

161

Detection of Spinel ZnIn2O4 Formed as Nanostructures in ZnOW. Sato, S. Komatsuda, Y. Yamada and Y. Ohkubo
Phys. Rev. B, 90 (2014) 235204.
The Effect of hot DMSO Treatment on the γ-ray-induced Grafting of Acrylamide onto PET Films
N. Rahman, N. Sato, M. Sugiyama, Y. Hidaka, H. Okabe and K. Hara
Polym. J., 46 (2014) 412-421.
Research activities on JASMIN: Japanese and American Study of Muon Interaction and Neutron Detection
H. Nakashima, N.V. Mokhov, Y. Kasugai, N. Matsuda, Y. Iwamoto, Y. Sakamoto, D. Boehnlein, A. Leveling, K.
Vaziri, R. Coleman, D. Jensen, E. Ramberg, A. Soha, T. Sanami, H. Matsumura, M. Hagiwara, A. Toyoda, H. Iwase,
H. Hirayama, T. Nakamura, S. Sekimoto, H. Yashima, T. Kajimoto, N.Shigyo, K. Ishibashi, N. Nakao, N. Kinoshita,
K. Oishi, H.S. Lee and K. Niita
Progress in Nuclear Science and Technology, 4 (2014) 191-196.
Novel Monolayer Shields of a Neutron Powder Diffractometer SPICA at BL09 of J–PARC
M. Kawai, M. Yonemura, S. Torii, T. Muroya, K. Mori, T. Fukunaga, K. Okuno, K. Takeda, K. Niita and
T. Kamiyama
Progress in Nuclear Science and Technology, 4 (2014) 156-159.
Measurement and Analysis of Neutron and Photon dose Rate in Concrete Shield of 120-GeV Proton Accelerator
Facility
K. Oishi, K. Kosako, Y. Kasugai, N. Matsuda, H. Yashima, S. Sekimoto, H. Matsumura, A. Toyoda, H, Iwase,
N. Mokhov, A. Leveling, D. Boehnlein, K. Vaziri, H. Nakashima and Y. Sakamoto
Progress in Nuclear Science and Technology, 4 (2014) 197-200.
Activation Detector Measurements at the Hadron Absorber of the NuMI Neutrino Beamline at Fermilab
N. Matsuda, Y. Kasugai, H. Matsumura, H. Iwase, A. Toyoda, H. Yashima, S. Sekimoto, K. Oishi, Y. Sakamoto,
H. Nakashima, T. Nakamura D. Boehnlein, G. Lauten, A. Leveling, N. Mokhov and K. Vaziri
Progress in Nuclear Science and Technology, 4 (2014) 337-340.
Radionuclides in the Cooling Water Systems for the NuMI Beamline and the Antiproton Production Target Station
at Fermilab
H. Matsumura, S. Sekimoto, H. Yashima, A. Toyoda, Y. Kasugai, N. Matsuda, K. Oishi, K. Bessho, Y. Sakamoto,
H. Nakashima, D. Boehnlein, G. Lauten, A. Leveling, N. Mokhov and K. Vaziri
Progress in Nuclear Science and Technology, 4 (2014) 372-375.
Comparison of Activity among Fluorescent Lamps and Light Emitting Diodes Lamps Exposed to Secondary Particles
in Accelerator Rooms
A. Toyoda, H. Matsumura, K. Masumoto, S. Sekimoto, H. Yashima, N. Matsuda, Y. Kasugai, Y. Sakamoto, H.
Nakashima, G. Lauten, A. Leveling, N. Mokhov, K. Vaziri, K. Oishi, M. Kuroyanagi, F. Nobuhara and K. Takahashi
Progress in Nuclear Science and Technology, 4 (2014) 384-387.
Reflectivity Enhancement in Titanium by Ultrafast XUV Irradiation
F. Bencivenga, E. Principi, E. Giangrisostomi, R. Cucini, A. Battistoni, F. D. Amico, A. D. Cicco, S. D. Fonzo, A.
Filipponi, A. Gessini, R. Gunnella, M. Marsi, L. Properzi, M. Saito and C. Masciovecchio
Sci. Rep., 4 (2014) 4952.
Neutron Diffraction Studies on Structural Effect for Ni-doping in LiCo1–xNixO2
D. S. Adipranoto, T. Ishigaki, A. Hoshikawa, K. Iwase, M. Yonemura, K. Mori, T. Kamiyama, Y. Morii and M.
HayashSolid State Ionics, 262 (2014) 92-97.

162

Visualization of Conduction Pathways in a Lanthanum Lithium Titanate Superionic Conductor Synthesized by Rapid
Cooling
K. Mori, S. Tomihira, K. Iwase and T. Fukunaga
Solid. State. Ionics., 268 (2014) 76-81.
Advanced Biological Treatment of Groundwater with Elevated Concentration of Arsenic and Ammonium
Y. Fujikawa, P. D Hung, K. Furukawa and A. Hashiguchi
The 20th Symposium on Soil and Groundwater Contamination and Remediation, 20 (2014) 136-140.
Elution Characteristics of Radioactive Materials in Heat-treated Soil (in Japanese)
M. Ikegami, Y. Takase, S. Fukutani, M. Yoneda, Y. Shimada and Y. Matsui
The 20th Symposium on Soil and Groundwater Contamination and Remediation, 20 (2014) 545-547.
Measurement of Air dose Rates Over a Wide Area Around the Fukushima Dai-ichi Nuclear Power Plant Through a
Series of Car-borne Surveys
M. Andoh, Y. Nakahara, S. Tsuda, T. Yoshida, N. Matsuda, F. Takahashi, S. Mikami, N. Kinouchi, T. Sato,
M. Tanigaki, K. Takamiya, N. Sato, R. Okumura, Y. Uchihori and K. Saito
J. Environ. Radioact., 139 (2015) 266-280.
U/238U Isotopic Ratio in Plant Samples from Fukushima Prefecture
Y. Shibahara, T. Kubota, T. Fujii, S. Fukutani, T. Ohta, K. Takamiya, R. Okumura, S. Mizuno and H. Yamana
J. Radioanal. Nucl. Chem., 303 (2015) 1421-1424.

235

Fe Polarization-Dependent Synchrotron M&oumlssbauer Spectroscopy Using a Diamond Phase Plate and an Iron
Borate Nuclear Bragg Monochromator
T. Mitsui, Y. Imai, R. Masuda, M. Seto and K. Mibu
J. Synchrotron Rad., 22 (2015) 427-435.
57

A Model Survey Meter Using Undoped Poly (Ether Sulfone)
H. Nakamura, Y. Shirakawa, M. Kanayama, N. Sato, H. Kitamura and S. Takahashi
Nucl. Instrum. Methods. Phys. Res. A, 780 (2015) 127.
Proceedings
Behavior of Cesium and Strontium in Waste Incineration
H. Aoki, K. Oshita, S. Fukutani, K. Shiota, T. Fujimori and M. Takaoka
8th i-CIPEC, Hang Zhou, China (2014).
Observation of Multiferroicity in GaFeO3 by Mössbauer Spectroscopy
S. Nakamura, Y. Kobayashi, S. Kitao, M. Seto and A. Fuwa
Int. Conf. on Strongly Correlated Systems 2014 (J. Phys. Conf. Ser. 592), Grenoble, France (2014) 12122.
Comparison of Solvent Power of N-PD and 2-PD toward Stereoregular Isotactic PAN
M. Minagawa, M. Shimuzu, T. Katoh, N. Sato and T. Matsuyama
The Fiber Society 2014 Spring Annual Meeting and Technical Conference, Liberec, Czech(May. 21-23, 2014) 107-108.
Reviews
Structures and Ion Conduction Pathways of Amorphous Lithium Ion Conductors (in Japanese )K. Mori, T. Fukunaga and Y. Onodera
HAMON, 24 (2014) 267-272.

163

Metal Nano Particles Fabrication under High Energy Irradiation Fields (in Japanese)
F. HoriMaterials Science & Technology, 84 (2014) 50.
Numerical Investigation Suggested for Brilliancy of Jewels as Detection of Scattered Light; (1) Estimation of Cut
Diamonds Considering Light Source and Observer (in Japanese )A. Kawaguchi
Yamanashi-Kenma-Houshoku-Shinbun, 672 (2015) 6.
5. Geochemistry and Environmental Science
PapersMeasurement of Large Negative Reactivity of an Accelerator-Driven System in the Kyoto University Critical
Assembly
A. Sakon, K. Hashimoto, M. A. B. Maarof, M. Kawasaki, W. Sugiyama, C.H. Pyeon, T. Sano, T. Yagi and T. Ohsawa
J. Nucl. Sci.Technol., 51 (2014) 116-126.
A Study on Redox Sensitive Elements in the Sediments at Dredged Trenches in Tokyo Bay by Instrumental Neutron
Activation Analysis
T. Yamagata, K. Shozugawa, R. Okumura, K. Takamiya and M. Matsuo
J. Radioanal. Nucl. Chem., 303 (2015) 1179-1183.
Bacterial Diversity in Biological Filtration System for the Simultaneous Removal of Arsenic, Iron and Manganesefrom Grouondwater
R. T. Chhetri, I. Suzuki, T. Fujita, M. Takeda, J. Koizumi, Y. Fujikawa, A. Minami, T. Hamasaki and M. Sugahara
J. Water. Environ. Technol., 12 (2014) 135-149.
Proposal of Simplified Storng Ground Motion Prediction Method for Synthetic Procedure Using Fault Model
Reflecting Nonlinear Site Effect
T. Ikeda, K. Konagai, K. Kamae, K. Irikura, T. Kiyota and K. Meguro
Japan Society of Civil Engineers, Vol.70, No. 4 (2014) 252-262.
Elution Characteristics of Cs and Sr in Heat-treated Soil (in Japanese)
M. Ikegami, Y. Takase, T. Kometani, M. Yoneda, Y. Shimada, Y. Matsui and S. Fukutani
Journal of Japan Society of Civil Engineers, Ser. G (Environmental Research), 70(7) (2014) 203-208.
Change of Leaching Characteristics of Cs and Sr from Soil by Wet and Dry Cycles (in Japanese)
T. Kometani, M. Yoneda, Y. Shimada, Y. Matsui, S. Fukutani and M. Ikegami
The 20th Symposium on Soil and Groundwater Contamination and Remediation, 20 (2014) 652-656.
Stratigraphy of the Tetori Group and the Jinzu Group (new name) in Gifu and Toyama Prefectures, Central Japan(in Japanese)
M. Matsukawa, M. Fukui, Y. Ogawa, T. Tano, K. Koarai, H. Ohira and K. Hayashi
The Journal of the Geological Society of Japan, 120 (2014) 147-164.
Rapid Survey of Four Asp Isomers in Disease-Related Proteins by LC-MS Combined with Commercial Enzyme
H. Maeda, T. Takata, N. Fujii, H. Sakaue, S. Nirasawa, S. Takahashi, H. Sasaki and N. Fujii
Anal. Chem., 87 (2015) 561-568.
Tetrakis (p-carboranylthio- tetrafluorophenyl) Chlorin (TPFC): Application for Photodynamic Therapy and Boron
Neutron Capture Therapy
R. Hiramatsu, S. Kawabata, H. Tanaka, Y. Sakurai, M. Suzuki, K. Ono, S. Miyatake, T. Kuroiwa, E. Hao, M. Graca
and H. Vicente
J. Pharm. Sci., 104 (2015) 962-970.

164

Proceedings
Slab-derived Noble Gases and Halogens with a Sedimentary Pore-fluid Signature
H. Sumino, M. Kobayashi, A. Shimizu, L. Jepson, D. Chavrit, C. Toyama, J. Kimura, Y. Muramatsu, R. Burgess and
C.J. Ballentine
Geofluid-3: Nature and Dynamics of Fluids in Subduction Zones, Tokyo, Japan (2014) 3.
Elucidation of the Uptake Route of Radionuclides in Deciduous and Coniferous Trees Using Radio Cesium andRadio Potassium in Annual Tree Rings
T. Ohta, Y. Mahara, H. Ogawa, A. Kumata, R. Fujinaga, A. Nishi and T. Igarashi
Proc. 15th workshop on Environmental Radioactivity, Tsukuba, Japan (2014) 228-232.
Noble Gases in the Chelyabinsk Meteorite
M.K. Haba, H. Sumino, K. Nagao, H. Mikouchi, M. Komatsu and M.E. Zolensky
The 45th Lunar and Planetary Science Conference, Texas, USA (2014) 1732.
The Origin of H2O-rich Fluids in Mantle Wedge Peridotites Revealed by Halogens and Noble Gases
M. Kobayashi, H. Sumino, K. Nagao, S. Ishimaru, S. Arai, M. Yoshikawa, T. Kawamoto, Y. Kumagai
And T. Kobayashi
Geofluid-3: Nature and Dynamics of Fluids in Subduction Zones, Tokyo, Japan (Apr. 28- May2, 2014) 21.
Difference in Removal Rate of Arsenite and Arsenate from Groundwater in Biological Filtration Systems- Resultsof on-site Voltammetric Analysis and XAFS Analysis
Y. Fujikawa, P. Lewtas, S. Tani, K. Takada, Ph.D. Hung, T. Homma and H. Ozaki
ICAEC2014, Bangkok (Nov. 24-26, 2014) 147.
Reviews
Analysis of Environmental Samples Using Synchrotron Radiation: Speciation of Elements by XAFS (in Japanese)
Y. Fujikawa
Journal of Environmental Conservation Engineering, 43(4) (2014) 220-225.
6. Life Science and Medical Science
PapersThe Structure of a Deoxygenated 400 kDa Haemoglobin Reveals Ternary- and Guaternary-structural Changes of
Giant Haemoglobins
N. Numoto, T. Nakagawa, R. Ohara, T. Hasegawa, A. Kita, T. Yoshida, T. Maruyama, K. Imai, Y. Fukumori and
K. MikiActa Cryst., D 70 (2014) 1823-1831.
Pilot Clinical Study of Boron Neutron Capture Therapy for Recurrent Hepatic Cancer Involving the Intra-arterial
Injection of a (10) BSH-containing WOW Emulsion
H. Yanagie, S. Higashi, K. Seguchi, I. Ikushima, M. Fujihara, Y. Nonaka, K. Oyama, S. Maruyama, R. Hatae, M.
Suzuki, S. Masunaga, T. Kinashi, Y. Sakurai, H. Tanaka, N. Kondo, M. Narabayashi, T. Kajiyama, A. Maruhashi,
K. Ono, J. Nakajima, M. Ono, H. Takahashi and M. Eriguchi
Appl. Radiat. Isot., 88 (2014) 32-37.
Design and Synthesis of 8-Hydroxyquinoline –based Radioprotective Agents
S. Ariyasu, A. Sawa, A. Morita, K. Hanaya, M. Hoshi, I. Takahashi, B. Wang and S. Aoki
Bioorg. Med. Chem., 22 (2014) 3891.

165

Impact of DNA Repair Pathways on the Cytotoxicity of Piperlongumine in Chicken DT40 Cell-lines
S. Okamoto, T. Narita, H. Sasanuma, S. Takeda, S. Masunaga, T. Bessho and K. Tano
Genes Cancer, 5 (2014) 285-292.
Safety and Effectiveness of Stereotactic Body Radiotherapy for a Clinically Diagnosed Primary Stage I Lung Cancer
Without Pathological Confirmation
K. Sakanaka, Y. Matsuo, Y. Nagata, S. Maki, K. Shibuya, Y. Norihisa, M. Narabayashi, N. Ueki, T. Mizowaki and
M. Hiraoka
Int. J. Clin. Oncol., 19(5) (2014) 814-821.
In vitro Amyloidogenic Peptides of Galectin-7: Possible Mechanism of Amyloidogenesis of Primary Localized
Cutaneous Amyloidosis
K. Ono, E. Fujimoto, N. Fujimoto, M. Akiyama, T. Satoh, H. Maeda, N. Fujii and S. Tajima
J. Biol. Chem., 289 (2014) 29195-29207.
Inflammation as well as Angiogenesis may Participate in the Pathophysiology of Brain Radiation Necrosis
E. Yoritsune, M. Furuse, H. Kuwabara, T. Miyata, N. Nonoguchi, S. Kawabata, H. Hana Hayasaki, T. Kuroiwa,
K. Ono, Y. Shibayama and S. Miyatake
J. Radiat. Res., 55 (2014) 803-11.
Emerging Issues in RadioGenic Cataracts and Cardio Vascular Disease
N. Hamada, Y. Fujimichi, T. Iwasaki, N. Fujii, M. Furuhashi, E. Kubo, T. Minamino, T. Nomura and H. SatoJ. Radiat. Res., 55 (2014) 831-846.
X-ray Structure Determination and Deuteration of Nattokinase
Y. Yanagisawa, T. Chatake, S. Naito, T. Ohsugi, C. Yatagai, H. Sumi, A. Kawaguchi, K. Chiba-Kamosida, M. Ogawa,T. Adachi and Y. Morimoto
J. Synchrotron Rad., (2014) 875-879.
Comparison of Effect of Gamma Ray Irradiation on Wild-type and N-terminal Mutants of αA-crystallin
S. Ramkumar, N. Fujii, N. Fujii, B. Thankappan, H. Sakaue, K. Ingu, K. Natarajaseenivasan and K. Anbarasu
Mol Vis., 20 (2014) 1002-1016.
The BRCA2 Gene is a Potential Molecular Target during 5-fluorouracil Therapy in Human Oral Cancer Cells
Y. Nakagawa, A. Kajihara, A. Takahashi, N. Kondo, E. Mori, T. Kirita and T. Ohnishi
Oncol. Rep., 31 (2014) 2001-2006.
Crystal Structure of Phosphopantothenate Synthetase from Thermococcuskodakarensis
A. Kishimoto, A. Kita, T. Ishibashi, H. Tomita, Y. Yokooji, T. Imanaka, H. Atomi and K. Miki
PROTEINS: Structure, Function and Bioinformatics, 82 (2014) 1924-1936.
Effects of Carotenoids on Damage of Biological Lipids Induced by Gamma Irradiation
T. Saito and N. Fujii
Radiat. Phys. Chem., 98 (2014) 57-63.
Significance of Fractionated Administration of Thalidomide Combined with γ-ray Irradiation in Terms of Local
Tumor Response and Lung Metastasis
S. Masunaga, Y. Sanada, T. Moriwaki, K. Tano, Y. Sakurai, H. Tanaka, M. Suzuki, N. Kondo, M. Narabayashi,
T. Watanabe, Y. Nakagawa, A. Maruhashi and K. Ono
World. J. Oncol., 5 (2014) 155-165.

166

New Quaternary Arsenide Oxides with Square Planar Coordination of Gold(I) – Structure,197Au M&oumlssbauer
Spectroscopic、 XANES and XPS Characterization of Nd10 Au3 As8 O10 and Sm10 Au3 As8 O10
T. Bartsch, O. Niehaus, D. Johrendt, Y. Kobayashi, M. Seto, P. M. Abdala, M. Bartsch, H. Zacharias, R. Hoffmann,
B. Gerke, U. Rodewald and R. P&oumlttgen
Dalton Trans., 44 (2015) 5854-5866.
Corrosion of Copper in Water and Colloid Formation under Intense Radiation Field
K. Bessho, Y. Oki, N. Akimune, H. Matsumura, K. Masumoto, S. Sekimoto, N. Osada, N. Kinoshita, H. Monjushiro
and S. Shibata
J. Radioanal. Nucl. Chem., 303 (2015) 1117-1121.
Copper Isotope Effect in Serum of Cancer Patients. A Pilot Study
P. Telouk, A. Puisieux, T. Fujii, V. Balter, V. Bondanese, A. P. Morel, G. Clapisson, A. Lamboux and
F. AlbaredeLBARÈDE
Matallomics, 7 (2015) 299-308.
Proceedings
Crystal Structure of Archaeal Phosphopantothenate Synthetase
A. Kita, A. Kishimoto, T. Ishibashi, H. Yomita, Y. Yokooji, T. Imanaka, H. Atomi and K. Miki
The 23rd Congress and General Assembly of the International Union of Crystallography, Montreal (Aug. 5-12, 2014)
C455.
Partial Oxygen-dissociation of Crystalline Giant Hemoglobin
N. Numoto, T. Nakagawa, A. Kita, N. Ito, Y. Fukumori and K. Miki
The 23rd Congress and General Assembly of the International Union of Crystallography, Montreal (Aug. 5-12, 2014)
C474.
Weak Interaction of an Inhibitor in the 20S Proteaspome
T. Murakami, H. Yamaguchi, U. Bahrudin, A. Kita, U. Hisatome, Y. Saeki, K. Tanaka, M. Unno and Y. Morimoto
The 23rd Congress and General Assembly of the International Union of Crystallography, Montreal (Aug. 5-12, 2014)
C487.
Rapid Analysis of D-amino acids in Proteins Using LC-MS
N. Fujii
Origins 2014, Nara, Japan (July 6-11, 2014) 14.
Protein Aggregation and Racemization of Amino Acids
N. Fujii, N. Fujii, T. Takata, H. Maeda and H. Sakaue
Japan-Hungary Joint Seminar "Mechanism and Regulation of Aberrant Protein Aggregation", Osaka, Japan(Nov. 18-20, 2014).
The Hunt for D-aspartyl Endopeptidase in Various Living Things:Vertebrates, Aquatic Animals and Plants
T. Kinouchi and N. Fujii
The 2nd International Conference of D-Amino Acid Research IDAR2014, Tochigi, Japan (Sept. 2-5, 2014) 16.
Oxidation and Racemization of Rat Lens Crystallins by gamma Irradiation
I. Kim, T. Saito and N. Fujii
The 2nd International Conference of D-Amino Acid Research IDAR2014, Tochigi, Japan (Sept. 2-5, 2014) 29.
Isomerizatons of Aspartyl Residues in Lens Crystallins from Age-related Cataracts
T. Takata, H. Sakaue and N. Fujii
The 2nd International Conference of D-Amino Acid Research IDAR2014, Tochigi, Japan (Sept. 2-5, 2014) 69.

167

Inversion of Aspartyl Residue Disturbs Assembly of Crystallin in Human Cataract Lens
H. Sakaue, T. Takata, N. Fujii, H. Sasaki and N. Fujii
The 2nd International Conference of D-Amino Acid Research IDAR2014, Tochigi, Japan (Sept. 2-5, 2014) 77.
A Novel Rapid Comprehensive Analysis of D-amino Acids in Cataract Lens Proteins Using LC-MS
N. Fujii
The 2nd International Conference of D-Amino Acid Research IDAR2014, Tochigi, Japan (Sept. 2-5, 2014) 28.
Analysis of Aspartyl Isomers in Skin Protein by LC-MS/MS
Y. Suzuki, N. Fujii and H. Sakaue
The 2nd International Conference of D-Amino Acid Research IDAR2014, Tochigi, Japan (Sept. 2-5, 2014) 78.
Books
Protein Modifications by Aging, Gamma-ray and UV Irradiation, and their Rapid Survey. Chap 16， Biomolecules
Under Extreme Environments, CSJ Current Review17 (in Japanese)
N. Fujii
Kagakudojin, (2014).
Cancer Treatments Targeting Aduptive Responces to Oxydative Stress
Medicine of Oxidative Stress
H. Nagasawa
SHINDAN TO CHIRYO SHA (2014).
Isomerizatons of Aspartyl Residues in Lens Crystallins from Age-related Cataracts
N. Fujii, T. Takata, N. Fujii and H. Sasaki
Asia ARVO, Yokohama, Japan (Feb. 16-19, 2015).
New Enzyme-Targeting Radiosensitization Treatment KORTUC, its Basis and Clinical Application cf. KORTUC(Kochi Oxydol-Radiation Therapy for Unresectable Carcinomas) (in Japanese)
S. Masunaga
Shinohara Publisher Inc, (2015).
New Developments in Tryptophan Research
A. Shimada and I. Otsuka
Nova Science Publishers, (2015).
Reviews
Current Status of Radiation Biology (in Japanese)
S. Masunaga
Jastro Newsletter, 112 (2014) 38.
Intrinsic and Extrinsic Factors Influencing the Radio-sensitivity (in Japanese)
S. Masunaga
Jastro Newsletter, 112 (2014) 42-44.
D-amino Acid as a Biomarker for the Photo-aging Mechnism (in Japanese)
N. Fujii
Journal of Clinical and Experimental Medicine (IGAKU NO AYUMI), 248 (2014) 602-607.

168

New Analysis of Aspartyl Isomers in Cataractous Lens Proteins (in Japanese)
N. Fujii and N. Fujii
The Journal of the Japanese Society for Cataract Research, 26 (2014) 33-36.
Abnormal Aggregation of Proteins Induced by Biologically Uncommon D-aspartyl Residues and Age-relatedDiseases (in Japanese)
N. Fujii
Vitamins, 88 (2014) 419-424.
From the Viewpoint of Tumor Biology (Biology for Tumor Therapy) (in Japanese)
S. Masunaga
Radioisotopes, 64 (2015) 69-79.
OthersA Method for the Detection of Iron(II) Ion by a Novel Selectove Fluorescence Probe (in Japanese)
H. Nagasawa and T. Hirayama
Japanese Patent Application No. 2014-007140.
A New Diagnostic Agent for Hypoxia Related Ocular Diseases (in Japanese)
S. Fukuda, T. Oshika, K. Okuda and H. Nagasawa
Japanese Patent Application No. 2014-200397.
7. Neutron Capture Therapy
PapersOverview of the Re-initiation of BNCT Clinical Studies at the University of Tsukuba
T. Aihara, H. Kumada, T. Wada, H. Ishikawa, N. Fukumitsu, K. Oonishi, K. Tanaka, M. Mizumoto, H. Numajiri, K.
Nakai, T. Yamamoto, T. Sakoda, A. Hara, A. Matsumura, M. Suzuki and H. Sakurai
16th Neutron Capture Therapy, (2014) 86-87.
A Simple Strategy to Decrease the Incidence of Fatal Carotid Blowout Syndrome after BNCT for Head and Neck
Cancers (in Japanese)
T. Aihara, N. Morita, N. Kamitani, H. Kumada, K. Oonishi, M. Suzuki, J. Hiratsuka and H. Sakurai
16th Neutron Capture Therapy, (2014) 171-172.
Synthesis and in Vitro Evaluation of ThiododeCaborated α，α-cycloalkylamino Acids for the Treatment of Malignant
Brain Tumors by Boron Neutron Capture Therapy.
Y. Hattori, S. Kusaka, M. Mukumoto, M. Ishimura, Y. Ohta, H. Takenaka, K. Uehara, T. Asano, M. Suzuki, S.
Masunaga, K. Ono, S. Tanimori and M. Kirihata
Amino Acids, 46 (2014) 2715-2720.
Higher Order Mode Analyses of Power Spectral Density and Feynman-alpha Method in Accelerator Driven Systemwith Periodically Pulsed Spallation Neutron Source
T. Yamamoto
Ann. Nucl. Energy., 66 (2014) 63-73.
An NDT Study of a Boron Tracedrug UTX-51 for Glycated BSA as an AGE Model
R. Tada, Y. Uto, S. Masunaga, Y. Kinashi, K. Ono and H. Hori
Anticancer Res, 34 (2014) 4503-4507.

169

Effect of Terrigenic He Components on Tritium-helium Dating: A Case Study of Shallow Groundwater in the Saijo
BasinY. Mahara, T. Ohta, N. Morikawa, T. Nakano, M. Tokumatsu, S. Fukutani and T. Igarashi
Appl. Geochem., 50 (2014) 142-149.
Pilot Clinical Study of Boron Neutron Capture Therapy for Recurreced Hepatic Cancer using Intra-Arterial Injectionof 10BSH Entrapped WOW Emulsion
H. Yanagie, S. Higashi, K. Seguchi, I. Ikushima, M. Fujihara, K. Oyama, Y. Nonaka, S. Maruyama, R. Hatae, M.
Suzuki, S. Masunaga, T. Kinashi, Y. Sakurai, H. Tanaka, N, Kondo, T. Kajiyama, A. Maruhashi, K. Ono, J. Nakajima,
M. Ono, H. Takahashi and M. Eriguchi
Appl. Radiat. Isot., 88 (2014) 32.
BNCT for Advanced or Recurrent Head and Neck Cancer
T. Aihara, N. Morita, N. Kamitani, H. Kumada, K. Ono, J. Hiratsuka and T. Harada
Appl. Radiat. Isot., 88 (2014) 12-15.
Dose Estimation for Internal Organs during Boron Neutron Capture Therapy for Body-trunk Tumors
Y. Sakurai, H. Tanaka, M. Suzuki, S. Masunaga, Y. Kinashi, N. Kondo, K. Ono and A. Maruhashi
Appl. Radiat. Isot., 88 (2014) 43-45.
Boron Neutron Capture Therapy as New Treatment for Clear Cell Sarcoma: Trial on Different Animal Model
T. Andoh, T. Fujimoto, T. Sudo, M. Suzuki, Y. Sakurai, T. Sakuma, H. Moritake, T. Sugimoto, T. Takeuchi,
H. Sonobe, A. L. Epstein, Y. Fukumori, K. Ono and H. Ichikawa
Appl. Radiat. Isot., 88 (2014) 59-63.
Gadolinium-loaded Chitosan Nanoparticles for Neutron-capture Therapy: Influence of Micrometric Properties of the
Nanoparticles on Tumor-killing Effect
H. Ichikawa, T. Uneme, T. Andoh, Y. Arita, T. Fujimoto, M. Suzuki, Y. Sakurai, H. Shinto, T. Fukasawa, F. Fujii
and Y. FukumoriAppl. Radiat. Isot., 88 (2014) 109-113.
Study on Detecting Spatial Distribution of Neutrons and Gamma Rays Using a Multi-imaging Plate System
K. Tanaka, Y. Sakurai, S. Endo and J. Takada
Appl. Radiat. Isot., 88 (2014) 143-146.
Evaluation of Thermal Neutron Field Using a Cyclotron-based Neutron Source for Alpha Autography
H. Tanaka, Y. Sakurai, M. Suzuki, S. Masunaga, T. Mitsumoto, Y. Kinashi, N. Kondo, M. Narabayashi, Y. Nakagawa,
T. Watanabe, N. Fujimoto, A. Maruhashi and K.Ono
Appl. Radiat. Isot., 88 (2014) 153-156.
Spermidinium Closo-dodecaborate-encapsulating Liposomes as Efficient Boron Delivery Vehicles for Neutron
Capture Therapy
S. Tachikawa, T. Miyoshi, H. Koganei, M. E. El-Zaria, C. Viñas, M. Suzuki, K. Ono and H. Nakamura
Chem. Commun., 50 (2014) 12325.
Optimization of Biguanide Derivatives as Selective Antitumor Agents Blocking Adaptive Stress Responses in the
Tumor Microenvironment
K. Narise, K. Okuda, Y. Enomoto, T. Hirayama and H. Nagasawa
Drug Des. Devel. Ther., 8 (2014) 701.
Effect of Bevacizumab Combined with Boron Neutron Capture Therapy on Local Tumor Response and Lung
Metastasis
S. Masunaga, Y. Sakurai, K. Tano, H. Tanaka, M. Suzuki, N. Kondo, M. Narabayashi, T. Watanabe, Y. Nakagawa,
A, Maruhashi and K. Ono
Exp. Ther. Med, 8 (2014) 291-301.

170

Evaluation of Boron Content Liposome Modified Protein-transduction Domains for Boron Neutron Capture Therapy
M. Shirakawa, K. Nakai, F. Yoshida, A. Zaboronok, T. Yamamoto and A. Matsumura
Int. J. Emerg.Technol. Adv. Eng., 4 (2014) 074-9.
Tetrakis (p-Carboranylthio-Tetrafluorophenyl) Chlorin (TPFC):Application for Photodynamic Therapy and Boron
Neutron Capture Therapy
R. Hiramatsu, S. Kawabata, H. Tanaka, Y. Sakurai, M. Suzuki, K. Ono, SI. Miyatake, T. Kuroiwa, E. Hao and MG.
VicenteJ Pharm Sci., 104(3) (2014) 962-70.
Boron Carbide Particle as a Boron Compound for Boron Neutron Capture Therapy
T. Iwagami, Y. Ishikawa, N. Koshizaki, N. Yamamoto, H. Tanaka, S. Masunaga, Y. Sakurai, I. Kato, S. Iwai,
M. Suzuki and Y. Yura
J. Nucl. Med. Radiat. Ther., 5 (2014) .
Mockup Experiments on the Thorium-Loaded Accelerator-Driven System in the Kyoto University Critical Assembly
C. H. Pyeon, T. Yagi, K. Sukawa, Y. Yamaguchi and T. Misawa
Nucl. Sci. Eng., 177 (2014) 156-168.
A Case of Radiation-induced Osteosarcoma Treated Effectively by Boron Neutron Capture Therapy
G, Futamura, S, Kawabata, H. Siba, T, Kuroiwa, M. Suzuki, N. Kondo, K. Ono, Y. Sakurai, M. Tanaka, T. Todo and
S. Miyatake
Radiat. Oncol., 9 (2014) .
The Roles of Platelet-Derived Growth Factors and their Receptors in Brain Radiation Necrosis
T. Miyata, T. Toho, N. Nonoguchi, M. Furuse, H. Kuwabara, E. Yoritsune , S. Kawabata, T. Kuroiwa andSI. Miyatake
Radiat. Oncol., 11 (2014) .
Detection of γH2AX Foci in Mouse Normal Brain and Brain Tumor after Boron Neutron Capture Therapy
N. Kondo, H. Michiue, Y. Sakurai, H. Tanaka, Y. Nakagawa, T. Watanabe, M. Narabayashi, Y. Kinashi, M. Suzuki,
S. Masunaga and K. Ono
Rep. Prac. Oncol. Radiother., in press (2014) .
Atmospheric Direct Uptake of Radiocaesium into Trees from the Fukushima Nuclear Accident and its Fate
Y. Mahara, T. Ohta, H. Ogawa and A. Kumata
Scientific Report, 4 (2014).
Study of Neutron Irradiation on F82H Alloys by Mössbauer Spectroscopy
S.S. Huang, S. Kitao, Y. Kobayashi, T. Yoshiie, Q. Xu, K. Sato and M. Seto
J. Nucl. Mater., 456 (2015) 266.
Preliminary Study of MAGAT Polymer Gel Dosimetry for Boron-neutron Capture Therapy
S. Hayashi, Y. Sakurai, R. Uchida, M. Suzuki, S. Usui and T. Tominaga
J. Phys. Conf. Ser., 573 (2015).
Mössbauer Spectroscopy of the Magnetic-Field-Induced Ferroelectric Phase of CuFeO2
S. Nakamura, Y. Kobayashi, S. Kitao, M. Seto, A. Fuwa and N. Terada
J. Phys. Soc. Jpn., 84 (2015) 24719.

171

Cherenkov Counting of 90Sr and 90Y in Bark and Leaf Samples Collected Around Fukushima Daiichi Nuclear Power
Plant
T. Kubota, Y. Shibahara, S. Fukutani, T. Fujii, T. Ohta, M. Kowatari, S. Mizuno, K. Takamiya and H. Yamana
J. Radioanal. Nucl. Chem., 303 (2015) 39-46.
Theoretical and Experimental Study of the Vibrational Frequencies of UO 22+ and NpO22+ in Highly Concentrated
Chloride Solutions
T. Fujii, A. Uehara, Y. Kitatsuji and H. Yamana
J. Radioanal. Nucl. Chem., 303 (2015) 1015-1020.
Local Structures at In Impurity Sites in ZnO Probed by the TDPAC Technique
W. Sato, S. Komatsuda, Y. Yamada and Y. Ohkubo
J. Radioanal. Nucl. Chem., 303 (2015) 1201-1204.
Neutron Activation Analysis of Iron Meteorites
N. Shirai, Y. HIdaka, A. Yamaguchi, S. Sekimoto, M. Ebihara and H. Kojima
J. Radioanal. Nucl. Chem., 303 (2015) 1375-1380.
U 238U Isotopic Ratio in Plant Samples from Fukushima Prefecture
Y. Shibahara, T. Kubota, T. Fujii, S. Fukutani, T. Ohta, K. Takamiya, R. Okumura, S. Mizuno and H. Yamana
J. Radioanal. Nucl. Chem., 303 (2015) 1421-1424.

235

Chemical and Mineralogical Compositions of Two Grains Recovered from Asteroid Itokawa
M. Ebihara, N. Shirai and S. Sekimoto
Meteorit. Planet. Sci., 50 (2015) 243-254.
Development of KURAMA-II and its Operation in Fukushima
M. Tanigaki, R. Okumura, K. Takamiya, N. Sato, H. Yoshino, H. Yoshinaga, Y. Kobayashi, A. Uehara andH. Yamana
Nucl. Instrum. Meth. Phys. Res., 781 (2015) 57-64.
Optical Characteristics of Pure Poly (vinyltoluene) for Scintillation Applications
H. Nakamura, Y. Shirakawa, N. Sato, H. Kitamura, O. Shinji, K. Saito and S. Takahashi
Nucl. Instrum. Methods. Phys. Res. A, 770 (2015) 131.
Proceedings
Boron-containing Rare Earth Oxides Nanoparticles for Boron Neutron Capture Therapy
T. Nagasaki, R. Kawasaki, S. Masunaga, Y. Sakurai and K. Tomita
2014 MRS Spring Meeting & Exhibit, San Francisco, CA, USA (2014).
Fatal Carotid Blowout Syndrome after BNCT for Head and Neck Cancers
T. Aihara, N. Morita, N. Kamitani, H. Kumada, K. Ohnishi, H. Ishikawa, N. Fukumitsu, M. Suzuki, T. Harada
Y. Sakurai and J. Hiratsuka
The 11th Congress on Neytron Capture Therapy, Osaka, Japan (2014) 63.
Development of a Real-time Thermal Neutron Monitor and its Clinical Application
T. Aihara, N. Morita, N. Kamitani, H. Kumada, K. Ohnishi, H. Ishikawa, N. Fukumitsu, M. Suzuki, T. Harada
Y. Sakurai and J. Hiratsuka
The 11th Congress on Neytron Capture Therapy, Osaka, Japan (2014) 85.

172

Fatal Carotid Blowout Syndrome after BNCT for Head and Neck Cancers
T. Aihara, N. Morita, N. Kamitani, H. Kumada, K. Ohnishi, M. Suzuki, J. Hiratsuka, H. Sakurai and T. Harada
The 76th Annual Meeting of the Society of Practical Otolaryngology, Morioka, Japan (2014) 143.
Cyclotron-based Epithermal Neutron Source (C-BENS) for Boron Neutron Capture Therapy
H. Tanaka, Y. Sakurai, M. Suzuki, S. Masunaga, T. Mitsumoto, A. Maruhashi and K Ono
Asian Forum for Accelerators and Detectors2015, Hsinchu, (2015).
The Past, Present, and Future of the Reactor-based Neutron Source at Kyoto University Reactor
Y. Sakurai, H. Tanaka, T. Takata, N. Fujimoto, M. Suzuki, S. Masunaga, Y. Kinashi, N. Kondo, M. Narabayashi,
Y. Nakagawa, T. Watanabe, K. Ono and A. Maruhashi
The 2nd KURRI International Workshop on BNCT - Basic Science and Technology for BNCT -, Kyoto, Japan(Dec. 9-10, 2014).
The Dependency of CBE Factors on the Concentration of Administered Neutron Capture Agents in BNCTS. Masunaga, Y. Sakurai, H. Tanaka, K. Tano, M. Suzuki, N. Kondo, M. Narabayashi, T. Watanabe, Y. Nakagawa,
A. Maruhashi and K. Ono
The 2nd KURRI International Workshop on BNCT - Basic Science and Technology for BNCT - Kyoto, Japan(Dec. 9-10, 2014).
Melanoma-Targeting Boron Delivery System Using Kojic Acid-Carborane Conjugate
T. Nagasaki, R. Kawasaki, Y. Hattori, Y. Sakurai, H. Tanaka, S. Masunaga, K. Ono and M. Kirihata
The 2nd KURRI International Workshop on BNCT - Basic Science and Technology for BNCT -, kyoto, Japan(Dec. 9-10, 2014).
Development of Real Time Neutron Monitors for BNCT
H. Tanaka, Y. Sakurai, M. Suzuki, S. Masunaga, Y. Kinashi, K. Taki, T. Fujii, N. Fujimoto, T. Takata, T. Watanabe,
Y. Nakagawa, M. Narabayashi, N. Kondo, A. Maruhashi and K. Ono
The 2nd KURRI International Workshop on BNCT - Basic Science and Technology for BNCT -, Kyoto, Japan(Dec. 9-10, 2014).
Clinical Experiences of Boron Neutron Capture Therapy to Recurrenced Rectal Cancers
H. Yanagie, K. Oyama, R. Hatae, S. Maruyama, Y. Ohno, S. Kurokawa, Y. Nonaka, H. Sugiyama, Y. Furuya, K.
Taniike, M. Suzuki, S. Masunaga, T. Kinashi, Y. Sakurai, N. Kondo, M. Narabayashi, H. Tanaka, A. Maruhashi, K.
Ono, J. Nakajima, M. Ono, H. Takahashi and M. Eriguchi
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 56-57.
Boron Neutron Capture Therapy as New Treatment for Clear Cell Sarcoma: Trial on a Lung Metastasis Model ofClear Cell Sarcoma
T. Andoh, T. Fujimoto, M. Suzuki, T. Sudo, Y. Sakurai, H. Tanaka, I. Fujita, N. Fukase, H. Moritake, T. Sugimoto,T. Sakuma, H. Sasai, T. Akisue, M. Kirihata, Y. Fukumori, K. Ono and H. Ichikawa
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 79-80.
Examination of the Usefulness as the New Boron Compound of ACBC-BSH
G. Futamura, S. Kawabata, S. Miyatake, T. Kuroiwa, Y. Hattori, M. Kirihata, H. Tanaka, Y. Sakurai, S. Masunaga
and K. Ono
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 81-82.
Potential of Boron Neutron Capture Therapy for Malignant Peripheral Nerve Sheath Tumor
T. Fujimoto, T. Andoh, Y. Tokunaga, T. Sudo, I. Fujita, N. Fukase, T. Takeuchi, H. Sonobe, M. Inoue, T. Hirose,
T. Sakuma, S. Yamamoto, S. Atagi, Y. Sakurai, H. Ichikawa, K. Ono and M. Suzuki
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 90-91.

173

Feasible Evaluation of WOW Emulsion as Intra-arterial Boron Delivery Carrier for Neutron Capture Therapy to
Hepatocellular Carcinoma
H. Yanagie, T. Kajiyama, M. Fijiwara, R. Mizumachi, Y. Murata, Y. Sakurai, K. Mouri, A. Shinohara, T. Matsukawa,Y. Oomori, Y. Morishita, N. Dewi, M. Yanagawa, S. Higashi, I. Ikushima, K. Seguchi, K. Yokoyama, T. Iizuka, Y.
Nonaka, H. Sugiyama, Y. Furuya, Y. Sakurai, H. Tanaka, M. Suzuki, S. Masunaga, K. Oyama, T. Nakagawa, R.
Nishimura, K. Ono, M. Ono, J. Nakajima, M. Eriguchi and H. Takahashi
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 98-99.
Study on the Improvement of Depth dose Distribution Using Multiple-field Irradiation in Boron Neutron Capture
Therapy
N. Fujimoto, H. Tanaka, Y. Sakurai, N. Kondo, M. Narabayashi, Y. Nakagawa, T. Watanabe, Y. Kinashi,
S. Masunaga, A. Maruhashi, K. Ono and M. Suzuki
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
101-102.
A study of Effective dose for Tumor in BNCTY. Sakurai, H. Tanaka, N. Fujimoto, N. Kondo, M. Narabayashi, Y. Nakagawa, T. Watanabe, Y. Kinashi, M. Suzuki,
S. Masunaga, A. Maruhashi and K.Ono
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
104-105.
Experimental Trial of Measuring Spatial Distribution of Neutrons and Gamma Rays in BNCT Using Multi Imaging
Plate System
K. Tanaka, Y. Sakurai, S. Endo, H. Tanaka and J. Takada
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
109-110.
Alanine Dosimeter Response Characteristics for Charged Particles in BNCT
T. Kawamura, R. Uchida, H. Tsuchida, H. Tanaka and Y. Sakurai
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
115-116.
Study on the Accelerator-based Neutron Source Using Be(p,n) Reaction with Proton Energy of Lower than 30 MeV
H. Tanaka, Y. Sakurai, M. Suzuki, S. Masunaga, N. Fujimoto, Y. Kinashi, N. Kondo, T. Takata, T. Watanabe, M.
Narabayashi, A. Maruhashi and K.Ono
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
126-127.
The Improvement of the Energy Resolution in Epi-thermal Region of Bonner Sphere Using Boric Acid Solution
Moderator
H. Ueda, H. Tanaka and Y. Sakurai
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)148-149.
Clinical Results of Boron Neutron Capture Therapy for the Patients with Malignant Meningioma
S. Kawabata, S. Miyatake, G. Futamura, R. Hiramatsu, Y. Matsushita, M. Furuse, Y. Tamura, T. Kuroiwa, H. Tanaka,
Y. Sakurai, S. Masunaga, M. Suzuki and K.Ono
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
169-170.

174

Three in One: a Multifunctional Antitumor Sensitizer for Photodynamic, Boron Neutron Capture and Proton
Therapies
N. Miyoshi, S. K.Kundu, H. Tanaka, Y. Sakurai, M. Suzuki, A.V. Zaitsev, V.A. Ol’shevskaya, G.N. Rychkov,
K. Ono, V.N.Kalinin and A. A.Shtil
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
173-174.
Significance of Combined Treatment with Bevacizumab in Boron Neutron Capture Therapy in Terms of Local Tumor
Response and Lung Metastasis
S. Masunaga, Y. Sakurai, K. Tano, H. Tanaka, M. Suzuki, N. Kondo, M. Narabayashi, T. Watanabe, Y. Nakagawa,
A. Maruhashi and K. Ono
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
177-178.
Detection of Plasmid Strand Breaks in Boron Neutron Capture Reaction
E. Okamoto, K. Nakai, F. Yoshida, M. Miyakawa, Y. Yamamoto, H. Tanaka, Y. Sakurai, S. Masunaga, T. Yamamoto
and A. Matsumura
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 179.
Localized dose Delivering by Ion Beam Irradiation for Experimental Trial of Establishing Brain Necrosis Model
T. Takata, N. Kondo, Y. Sakurai, H. Tanaka, T. Hasegawa, K. Kume and M. Suzuki
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 184.
Experimental Trial of Establishing Brain Necrosis Mouse Model Using Proton Beam
N. Kondo, Y. Sakurai, T. Takata, H. Tanaka, N. Takai, K. Kume, T. Watanabe, T. Toho, S. Miyatake, M. Suzuki, S.
Masunaga and K. Ono
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014) 183-184.
Novel Multi-linked Mercaptoundecahydrododecaborate (BSH) Fused Cellpenetrating Peptide Accelerated Boron
Neutron Capture Therapy (BNCT)
H. Michiue, Y. Sakurai, N. Kondo, M. Kitamatsu, F. Bin, K. Nakajima, Y. Hirota, S. Kawabata, T. Nishiki, I. Ohmori,K. Tomizawa, S. Miyatake, K. Ono and H. MatsuiBook of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
187-188.
Kojic Acid Modified O-carborane/Hydroxypropyl-β-cyclo-dextrin Complex as Novel BNCT Drug for Melanoma
T. Nagasaki, R. Kawasaki, Y. Sakurai, S. Masunaga, K. Ono and M. Kirihata
Book of Abstracts for 16th International Congress on Neutron Capture Therapy, Helsinki (Jun. 14-19, 2014)
222-223.
Stimuli-responsive Drug Delivery System: Photoresponsive Gene Delivery System for Gene Therapy and Boron
Delivery System for Neutron Capture Therapy
T. Nagasaki
7th KIFEE International Symposium on Environment, Energy and Materials, Kyoto, Japan (Mar. 1-3, 2014).
Clinical Results of Boron Neutron Capture Therapy for Cutaneous Malignant Melanoma (in Japanese)
J. Hiratsuka, N. Kamitani, S. Sasaoka, Y. Sakurai and M. Suzuki
The 11th Congress on Neutron Capture Therapy, Osaka, Japan (Mar. 1-3, 2014) 69.
A Remodelling Study of the Reactor-based Irradiation Facility for Boron Neutron Capture Therapy at Kyoto
University Research Reactor InstituteY. Sakurai, T. Takata, H. Tanaka, N. Fujimoto, N. Kondo, Y. Nakagawa, T. Watanabe, M. Narabayashi, Y. Kinashi,
M. Suzuki, S. Masunaga, K. Ono and A. Maruhashi
Book of Abstracts for 14th Asia-Oceania Congress of Medical Physics & 12th South East Asia Congress of Medical
Physics (AOCMP/SEACOMP 2014), Ho Chi Minh City (Oct. 23-25, 2014) 126.

175

Significance of Administering Bevacizumab Combined with Boron Neutron Capture Therapy in Terms of Local
Tumor Control and Lung Metastatic Potential
S. Masunaga, Y. Sakurai, K. Tano, H. Tanaka, M. Suzuki , N. Kondo, M. Narabayashi, T. Watanabe, Y. Nakagawa,
A. Maruhashi and K. Ono
The 56th Annual Meeting of the American Society for Therapeutic Radiology and Oncology, San Francisco, USA(Sept. 14-17, 2014) 796.
Development of a Real-time Dosimeter for Boron Neutron Capture Therapy
H. Tanaka, Y. Sakurai, M. Suzuki, S. Masunaga, T. Takata, N. Fujimoto, K. Taki, A. Maruhashi and K. Ono
Book of Abstracts for the 7th Korea-Japan Joint Meeting on Medical Physics, Busan (Sept. 25-27, 2014) 141.
Clinical Application of Scintillator with Optical Fiber Detector as a Real-time Thermal Neutron Monitor during
Boron Neutron Capture Therapy
M. Ishikawa, K. Ono, A. Matsumura, T. Yamamoto, J. Hiratsuka, S. Miyatake, I. Kato, Y. Sakurai and H. Kumada
Book of Abstracts for the 7th Korea-Japan Joint Meeting on Medical Physics, Busan (Sept. 25-27, 2014) 129.
Advances in BNCT at Kyoto University Research Reactor Institute -from reactor-based BNCT to Accelerator-based
BNCT
Y. Sakurai
Book of Abstracts for the 7th Korea-Japan Joint Meeting on Medical Physics, Busan (Sept. 25-27, 2014) 26.
Preliminary Study of MAGAT Polymer Gel Dosimetry for Boron-neutron Capture Therapy
S. Hayashi, Y. Sakurai, R. Uchida, M. Suzuki, S. Usui and T. Tominaga
Book of Abstracts for 8th International Conference on 3D Radiation Dosimetry (IC3D Dose), Ystad(Sept. 4-7, 2014) 14.
Reviews
The First Case in the World of BNCT for a Patient with Head and Neck Cancer (in Japanese)
I. Kato and S. Kawabata
PET Journal, 25 (2014) 10-11.
Boron Neutron Capture Therapy (BNCT)
I. Ota and T. Kitahara
The Society of Practical Otolaryngology, 107 (2014) 937-946.
BNCT for Refractory Cancer
M. Suzuki
Electrical Review, 5 (2015) 10-11.
8. Neutron Radiography and Radiation Application
PapersNeutron Radiography and Numerical Simulation of Mixing Behavior in a Reactor for Supercritical Hydrothermal
Synthesis
K. Sugioka, K. Ozawa, S. Takami, T. Tsukada, T. Adschiri, K. Sugimoto, N. Takenaka and Y. Saito
AIChE J., 60 (2014) 1168.
A New Class of High-contrast Fe(II) Selective Fluorescent Probes Based on Spirocyclized Scaffolds for Visualizationof Intracellular Labile Iron Delivered by Transferrin
M. Niwa, T. Hirayama, K. Okuda and H. Nagasawa
Org. Biomol. Chem., 12 (2014) 6590-6597.

176

Estimation of Frost Formation by using Neutron Radiography : Estimation of Frost Deposition and Mass Transfer
Coefficient on Cold Flat Plate (in Japanese)
R. Matsumoto, T. Yoshimura, H. Umekawa, T. Ami, D. Ito and Y. Saito
Transactions of the Japan Societt of Refrigerating and Air Conditioning Engineers, Feb-31 (2014) 207.
Proceedings
Quantitative Estimation of Frost Formation on Plate-fin Tube Heat Exchanger by Neutron Radiography
R. Matsumoto, T. Yoshimura, H. Umekawa, T. Ami, D. Ito and Y. Saito
15th International Heat Transfer Conference, Kyoto, Japan (2014) 15.
Visualization of Water Accumulation Process in Polymer Electrolyte Fuel Cell using Neutron Radiography
H. Murakawa, K. Sugimoto, N. Kitamura, M. Sawada, H. Asano, N. Takenaka and Y. Saito
Proc. the 10th World Conference on Neutron Radiography, Grindelwald, Switzerland (Oct. 5-10, 2014) 175.
Visualization and Measurement of Adsorption/Desorption Process of Ethanol in Activated Carbon Adsorber
H. Asano, K. Murata, N. Takenaka and Y. Saito
Proc. the 10th World Conference on Neutron Radiography, Grindelwald, Switzerland (Oct. 5-10, 2014) 184.
Study on the Effect of Micro Porous Layer on Water Transport Phenomena in PEFC by Using Neutron Radiography
H. Murakawa, K. Sugimoto, N. Kitamura, H. Asano, N. Takenaka and Y. Saito
Proc. the 15th International Heat Transfer Conference (IHTC-15), Kyoto, Japan (Mar. 1-3, 2014) 15.
9. TRU and Nuclear Chemistry
PapersDensity Functional Theory Estimation of Isotope Fractionation of Fe, Ni, Cu and Zn Among Species Relevant toGeochemical and Biological Environments
T. Fujii, F. Moynier, J. B. Toft and F. Albare`deGeochim. Cosmochim. Acta, 140 (2014) 553-576.
Redox Equilibrium of the UO22+/UO2+ Couple in Li2MoO4–Na2MoO4 Eutectic Melt at 550ºC
T. Nagai, A. Uehara, T. Fujii, N. Sato, H. Kofuji, M. Myochin and H. Yamana
J. Nucl. Mater., 454 (2014) 159-163.
Coprecipitation Behaviors of Zr, Hf, and Th with Sm Hydroxide for Chemical Study of Element 104, Rf
Y. Kasamatsu, K. Toyomura, N. Shiohara, T. Yokokita, Y. Komori, A. Kino, T. Yoshimura, N. Takahashi, H. Haba,
Y. Kudou, H. Kikunaga, T. Mitsugashira, T. Ohtsuki, K. Takamiya and A. Shinohara
J. Nucl. Radiochem. Sci., 14 (2014) 7-11.
Analysis of Cesium Isotope Compositions in Environmental Samples by Thermal Ionization Mass Spectrometry- 1.
A Preliminary Study for Source Analysis of Radioactive Contamination in Fukushima Prefecture
Y. Shibahara, T. Kubota, T. Fujii, S. Fukutani, T. Ohta, K. Takamiya, R. Okumura, S. Mizuno and H. Yamana
J. Nucl. Sci. Technol., 51 (2014) 575-579.
Complex Light Source Composed from Subterahertz-wave Coherent Synchrotron Radiation and an Infrared
Free-electron Laser at the Laboratory for Electron Beam Research and Application
N. Sei, H. Ogawa, K. Hayakawa, T. Tanaka, Y. Hayakawa, K. Nakao, T. Sakai, K. Nogami and M. Inagaki
J. Opt. Soc. Am. B, 31 (2014) 2510.

177

Raman Spectroscopic Study on NpO2+-Ca2+ Interaction in Highly Concentrated Calcium Chloride
T. Fujii, A. Uehara, Y. Kitatsuji and H. Yamana
J. Radioanal. Nucl. Chem., 301 (2014) 293-296.
Solvent Extraction of Mo(V) and Mo(VI) from Hydrochloric Acid into Aliquat 336 Chloroform Solution
T. Yokokita, Y. Kasamatsu, K. Ooe, T. Yoshimura, N. Takahashi, Y. Komori and A. Shinohara
J. Radioanal. Nucl. Chem., 301 (2014) 751.
Undoped Polycarbonate for Detection of Environmental Radiation
H. Nakamura, Y. Shirakawa, H. Kitamura, N. Sato and S. Takahashi
Japanese Journal of Health Physics, 49 (2014) 98.
Blended Poly (Ether Sulfone) and Poly (Ethylene Naphthalate) as a Scintillation Material
H. Nakamura, Y. Shirakawa, N. Sato, H. Kitamura and S. Takahashi
Nucl. Instrum. Methods. Phys. Res. A, 759 (2014) 1.
Solvent Extraction Using Carrier-free Radiotracers of Mo and W from HCl and HCl/LiCl Solutions into Aliquat 336
T. Yokokita, K. Ooe, Y. Kasamatsu, T. Yoshimura, N. Takahashi, N. Shiohara, K. Takamiya, Y. Komori, Y. Kikutani,
A. Kino and A. Shinohara
J. Radioanal. Nucl. Chem., 303 (2015) 1091.
Comparison of the Decay Constants of 51Cr with Metal, Oxide, and Chromate Chemical States
H. Kikunaga, K. Takamiya, K. Hirose and T. Ohtsuki
J. Radioanal. Nucl. Chem., 303 (2015) 1581-1583.
Others
Structural analysis on Cations in Molten Sub-halide Systems: Fluoride Addition on UV-vis Spectra of
Neodymium cation in Molten Chlorides
H. Matsuura, A. Nezu and H. Akatsuka
Bulletin of Research Laboratory for Nuclear Reactors, 38 (2014) 12.
10. Health Physics and Waste Management
PapersUnraveling Low-level Gamma Radiation-responsive Changes in Expression of Early and Late Genes in Leaves of
Rice Seedlings at Litate Village, Fukushima
G. Hayashi, J. Shibata, T. Imanaka, K. Cho, A. Kubo, S. Kikuchi, K. Satoh, S. Kimura, S. Ozawa, S. Fukutani,
S. Endo, K. Ichikawa, G.K. Agrawal, S. Shioda, M. Fukumoto and R. Rakwal
J. Hered., 105 (2014) 723-738.
Estimation of β-ray dose in Air and Soil from Fukushima Daiichi Power Plant Accident
S. Endo, K. Tanaka, T. Kajimoto, N.T. Thanh, J.M. Otaki and T. Imanaka
J. Radiation Research, 55 (2014) 476-483.
Isotopic Compositions of Transuranic Nuclides Released by the Fukushima Dai-ichi Nuclear Power Plant Accident:with Emphasis on Cm Isotopes
M. Yamamoto, A. Sakaguchi, S. Ochiai and T. Imanaka
J. Radioanal. Nucl. Chem., 300 (2014) 1045-1052.

178

Development of On-site Heavy Metal Analysis Method and Technology for Selective Removal of Radioactive
Cesium in the Extracts of Designated Wastes (in Japanese)
Y. Fujikawa, H. Ozaki、P. Wei, H. Tsuno, A. Fujinaga, S. Taniguchi, R. Takanami, L. Paul and S. Sakurai
Proceedings of the 15th Workshop of Environmental Radioactivity, 15 (2014) 277-286.
Measurement of the Displacement Cross-section of Copper Irradiated with 125 MeV Protons at 12 K
Y. Iwamoto, T. Yoshiie, M. Yoshida, T. Nakamoto, M. Sakamoto, Y. Kuriyama, T. Uesugi, Y. Ishi, Q. Xu,
H. Yashima, F. Takahashi, Y. Mori and T. Ogitsu
J. Nucl. Mater., 458 (2015) 369-375.
Estimation of the Contribution of Short-lived Radioiodines to the Thyroid dose for the Public in Case of Inhalation
Intake Following the Fukushima Accident
S.M. Shinkarev, K.V. Kotenko, E.O. Granovskaya, V.N. Yatsenko, T. Imanaka and M. Hoshi
Radiat. Prot. Dosimetry., 164 (2015) 51-56.
Localization Estimation of Ionizing Radiation-induced Abasic Sites in DNA in the Solid State Using Fluorescence
Resonance Energy Transfer
K. Akamatsu, N. Shikazono and T. Saito
Radiat. Res., 183 (2015) 105-113.
Reviews
Decontamination Technology of Designated Wastes as Specified in Act on Special Measures Concerning theHandling of Radioactive Pollution &#8211; Procedures of the on-site Test (in Japanese)
Y. Fujikawa, H. Ozaki, H. Tsuno, A. Fujinaga, S. Taniguchi, R. Takanami, K. Fujiwara, S. Sakurai and L. Paul
Environmental & Sanitary Engineering Research, 28(3) (2014) 127-134.
11. Accelerator Physics
PapersPrecise Determination of Bromine in PP Resin Pellet by Instrumental Neutron Activation Analysis Using InternalStandardization
T. Miura, R. Okumura, Y. Iinuma, S. Sekimoto, K. Takamiya, M. Ohata and A. Hioki
J. Radioanal. Nucl. Chem., 303 (2015) 1417-1420.
Target Depth Dependence of Damage Rate in Metals by 150 MeV Proton Irradiation
T. Yoshiie, Y. Ishi, Y. Kuriyama, Y. Mori, K. Sato, T. Uesugi and Q. Xu
Nucl. Instrum. Meth. B., 342 (2015) 166-169.
Proceedings
Transport of Terahertz-wave Coherent Synchrotron Radiation with a Free-electron Laser Beamline at LEBRA
N. Sei, H. Ogawa, K. Hayakawa, T. Tanaka, Y. Hayakawa, K. Nakao, T. Sakai, K. Nogami and M. Inagaki
35th International Free Electron Laser Conference, Basel, Switzerland (Aug. 25-29, 2014) 541.
12. Others
PapersAu Electrodeposition at the Liquid-Liquid Interface: Mechanistic Aspects
A. Uehara, T. Hashimoto and R. A. W. Robert
Electrochim. Acta, 118 (2014) 26-32.

179

ASEAN Energy Security: An Indicator-based Assessment
K. Kanchana and H. Unesaki
Energy Procedia, 56 (2014) 163-171.
Risk Assessment of the Intake of Foods and Soil with the Radionuclides and the Air Radiation Dose after the
Fukushima Nuclear Disaster
A. Fujinaga, M. Yoneda and M. Ikegami
J. Eng. Gas. Turbine. Power, 136(8) (2014) 1-7.
Performance Evaluation of High-pressure MWPC with Individual Line Readout under Cf-252 Neutron Irradiation
K. Toh, T. Nakamura, K. Sakasai, K. Soyama and H. Yamagishi
J. Phys.: Conf. Ser., 528 (2014) 12045.
High Linear-energy-transfer Radiation can Overcome Radioresistance of Glioma stem-like Cells to Low Linearenergy-transfer Radiation
Y. Hirota, SI. Masunaga, N. Kondo, S. Kawabata, H. Hirakawa, H. Yajima , A. Fujimori, K. Ono, T. Kuroiwa andSI. Miyatake
J. Radiat. Res., 55 (2014) 75-83.
Effect of Ultraviolet and Radiation on Surface Wettability (in Japanese)
D. Ito, D. Nishi and Y. Saito
Japanease Journal of Multiphase Flow, 27-5 (2014) 555-561.
Hydrogen Trapping under the Effect of W-C Mixed Layers
N. Liu, J. Huang, K. Sato, Q. Xu, L. Q. Shi and Y. X Wang
Nucl. Fusion, 54 (2014) 33013.
Verification of Terahertz-wave Spectrophotometry by Compton Backscattering of Coherent Synchrotron Radiation
N. Sei and T. Takahashi
Phys. Lett. A, 378 (2014) 303-307.
Wide Dynamic Range Neutron Flux Monitor having Fast Time Response for the Large Helical Device
M. Isobe, K. Ogawa, H. Miyake, H. Hayashi, T. Kobuchi, Y. Nakano, K. Watanabe, A. Uritani, T. Misawa,
T. Nishitani, M. Tomitaka, T. Kumagai, Y. Mashiyama, D. Ito, S. Kono, M. Yamauchi and Y. Takeiri
Rev. Sci. Instrum., 85 (2014) 11.
Effect of Particle Size on Risk Assessment of Direct Soil Ingestion and Metals Adhered to Children’s Hands at
Playgrounds
M. Ikegami, M.Yoneda, T. Tsuji, O. Bannai and S. Morisawa
Risk Analysis, 34(9) (2014) 1677-1687.
αB- and βA3-crystallins Containing D-Aspartic Acids Exist in a Monomeric State
H. Sakaue, T. Takata, N. Fujii, H. Sasaki and N. Fujii
Biochim. Biophys. Acta., 1854 (2015) 1-9.
Proceedings
Bee and Wasp Stings: Analysis and Education in University
R. Kuroda, K. Yamamoto, T. Umekage, T. Iimoto and Y. Okubo
1st Asian Conf. on Safety and Education in Laboratory, The University of Tokyo, JAPAN (2014).

180

Framework of Radiological Safety for Natural Radioactive Materials (NORM/TENORM) and Related Education
T. Iimoto, R. Hayashi, R. Kuroda and K. Yamamoto
1st Asian Conf. on Safety and Education in Laboratory, The University of Tokyo,JAPAN (2014) .
Publishing Tool for Information of Environment, Health and Safety in Utokyo
H. Takizawa, Y. Okubo, T. Iimoto, R. Hayashi, R. Kuroda, K. Yamamoto and R. Dobashi
1st Asian Conference on Safety and Education in Laboratory, The University of Tokyo,JAPAN (2014) .
Basic Research on Radiation Tests Suitable For Nano-Satellites
T. Tomioka, H. Masui, M. Cho and K. Takamiya
65th Int. Astronautical Congress, Toronto, Canada (2014).
Books
Synergy in Supramolecular Chemistry
S. Aoki, M. Zulkefeli, Y. Hisamatsu and M. Kitamura
CRC, (2015).
Fundamentals of General, Organic, and Biological Chemistry (7th Edition) (in Japanese)
J. M. MuMurry, D. S. Ballantine, C. A. Hoeger and V. E. Peterson
Maruzen (2015).
Reviews
Development of a GPS-based Aautonomous Radiation Monitoring System, KURAMA (in Japanese)
M. Tanigaki
Chemical Engineering, VOL.59 No.3 (2014).
DNA Structures
T. Chatake
Crystallography in Japan (II), (2014) 218-219.
Development of a GPS-based Autonomous Radiation Monitoring System, KURAMA/KURAMA-II (in Japanese)
M. Tanigaki
Collections of the Removal Techniques of Radioactive Materials, (2015).

181

KURRI Progress Report 2014
Issued in July 2015
by the Research Reactor Institute, 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:
http://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep2014/ProgRep2014.html

Publication Team
ETO, Hiroko
IKEGAMI, Maiko
INOUE, Rintaro (Subchief)
KAWAGUCHI, Akio
MORI, Kazuhiro (Chief)
NAKAMURA, Hidehito
NAKATSUKA, Hiroto
NAKAYAMA, Chiyoko
OKUMURA, Ryo
SAITO, Takeshi
SAKURAI, Yoshinori (Subchief)
TAKAHASHI, Toshiharu
XU, Qiu
YAMAMOTO, Toshihiro
YOKOTA, Kaori