J-PARC
ANNUALREPORT2 O 1 4Vol.2: Materials and Life Science
Experimental Facility

MLF
ANNUALREPORTMaterials and Life Science Division
J-PARC Center
http://j-parc.jp/MatLife/en/index.html
J-PARC was jointly constructed and is now operated by the High Energy Accelerator
Research Organization (KEK) and the Japan Atomic Energy Agency (JAEA).

Comprehensive Research Organization for Science and Society
http://www.cross-tokai.jp/

J-PARC 16-01
KEK Progress Report 2015-5

MLF Annual Report 2014

PrefaceToshiji Kanaya
Division Head of Materials and Life Science Division, MLF
After the incident at the Hadron Facility on May 23rd, 2013, J-PARC/MLF resumed the beam operation for
the user program on February 17th, 2014. In JFY2014, MLF kept 300 kW steady operation with gas micro-bubbles injection in the neutron target. The scheduled beam time in JFY2014 was 166 days and the availability
was 69%. There were 895 unique users in that period and they presented 780 proposals.
In JFY2014, 18 instruments were under operation for neutron science. The construction of BL06 (VIN
ROSE), BL22 (RADEN) and BL23 (POLANO) at the neutron facility advanced, and VIN ROSE and RADEN proceeded to the commissioning phase (see Figure 1). As for the muon beam lines, the D1 and D2 instruments
were dedicated to the user programs and the U-line and the S-line were under commissioning (see Figure 2).
We had a fire accident in the muon area on January 16th, 2015, and the beam stopped until February 25th,
2015. We decided to carry the user experiments canceled due to the accident over to 2015A. After the accident, we reconsidered our protocols related to safety issues. The operation manuals have been reviewed. We
also introduced a new working standard protocol. According to the new protocol, all activities done in MLF
will be checked by each section. Any suspicious activities found by each section will be reviewed by the MLF
safety reviewing, which will be held during regular MLF meetings.

Figure 1. Layout of the neutron beam lines in MLF.

Figure 2. Layout of the muon beam lines in MLF.

PrefacePreface

MLF Annual Report 2014

Preface

Hideaki Yokomizo
Director, CROSS-Tokai
Four years have passed since CROSS-Tokai commenced operations in support of the user program at the
Public Beamlines at the Materials and Life Science Experimental Facility of J-PARC (J-PARC MLF).
As required by the “Promotion of Public Utilization of Specific Advanced Large-Scale Research Facilities”
legislation, under which CROSS was appointed and now operates, we are fully engaged in facility promotion
activities, such as operating a fair and open proposal selection system for the MLF Public Beamlines, providing high-quality user support and promoting facility utilization by both academic and industrial researchers.
During 2014, CROSS-Tokai supported the user program on six fully-operational Public Beamlines: BL01
4SEASONS, BL02 DNA, BL11 PLANET, BL15 TAIKAN, BL17 SHARAKU and BL18 SENJU. In addition, the construction work and commissioning continued on the seventh Public Beamline, BL22 RADEN, which will be available to users in 2015. Unfortunately, the user operations during the year were affected by the Muon Facility
incident and its aftereffects and the beamtime was suspended from mid-January to the end of March, 2015.
Special programs to promote facility utilization continued to operate successfully during 2014, such as
Trial Use and Elementary Strategy Initiative. Trial Use is a program that promotes the use of neutrons by firsttime or novice users from both the industrial and academic sectors, and Elementary Strategy Initiative is an
integrated strategic research program of the Japanese Government that aims to promote the developmentof innovative materials and alternative technologies in the target areas of permanent magnets, catalysis
and batteries, and electronic and structural materials. Moreover, Complementary Use is a program recommended to encourage and facilitate the complementary and collaborative use of pulsed neutrons (J-PARC
MLF), synchrotron radiation (SPring-8), and supercomputer (K computer), which was added to this programin 2014.
I hope this Annual Report would serve as a useful resource for anyone wishing to know more about thecurrent status of the MLF, its recent scientific achievements, the technical R&D projects that support the science program, and the operational details of our facility.
On behalf of the team at CROSS-Tokai, I extend a warm welcome to all researchers who wish to make useof the Public Beamlines at J-PARC MLF.

Research Center for Neutron Science and Technology, Comprehensive Research Organization for Science and Society
www.cross-tokai.jp

Contents
PrefaceResearch and Development Highlights
Site Occupancy of Interstitial Deuterium Atoms in Face-Centered Cubic Iron ···········································································

2

Simultaneous Characterization of Small-Angle Neutron Scattering and Bragg-Edge Transmission in Steel ···················

4

Relation between Vickers Hardness and Bragg-edge Broadening in Quenched Steel Rods ·················································

6

Study of the Structural Change in the Human Stratum Corneum Inducedby the Treatment of Surfactant Solutions ···········································································································································

9

Understanding the Mechanism of Gene Expression by Flexibility of the DNA Structure - Observationof Base-sequence Dependent DNA Dynamics by Quasi-elastic Neutron Scattering ························································· 11
QENS Study of Protein Dynamics in Glycerol and Water Mixture Measured on DNA ······························································· 13
Neutron Crystallography Reveals Two Protonation States of PcyA, a Bilin Reductase ····························································· 15
Phonon Anomaly in La1.5Sr0.5NiO4 ································································································································································· 18
Special Spin Density Distribution in T'-sturctured Cuprate Oxides Studied by μSR ·································································· 20
Magnetic Model in Multiferroics NdFe3(BO3)4 Investigated by Inelastic Neutron Scattering ················································· 22
Crystal Field Excitations in Breathing Pyrochlore Ba3Yb2Zn5O11 ········································································································ 24
Magnetic Excitations in the γ-FeMn Itinerant Electron Antiferromagnet ······················································································ 27
Anomalous Magnetic Response in the Overdoped Checkerboard Ordered Phaseof Layered Nickel Oxides Nd2-xSrxNiO4 ·················································································································································· 29
Nd-Substitution Effect on Metal–Nonmetal Transition in PrRu4P12 ·································································································· 32
Spin and Hole Dynamics in Carrier Doped Quantum Haldane Chain····························································································· 34
Intermultiplet Transitions in SmFe4P12 ························································································································································ 37
Observation of the Inside of a Lithium-ion Battery by Muonic X-ray ······························································································ 39
Systematic Studies on Muonium Production in Vacuum from Structured Silica Aerogel ······················································· 41
Neutron Activation Analysis using Pulsed Neutrons at J-PARC ANNRI ··························································································· 43
Neutron Reflectivity Measurement for Study of Water Permeability of Anticorrosive Ultrathin Film ································· 45
Measurement of Neutron Spatial Brightness from Coupled and Decoupled Para-hydrogen Moderators ······················· 48
Dynamic Structures of Superionic Conductors of MAg4I5 (M = K, Rb) by Inelastic Neutron Scattering ······························ 49
Progress in the Dynamic Nuclear Polarization on POLANO ··············································································································· 51
3He Neutron Spin Filter for POLANO ··························································································································································· 53

Estimation of Magnetic Field Distribution for Polarized Neutron Experiments ·········································································· 55

Neutron Source
Progress of the Neutron Source Section ···················································································································································· 60
Status of Proton Beam Commissioning at MLF ······································································································································· 62
Operation Experience for Mercury Target in 2014 ································································································································· 64
Development Status of the AuIC Decoupler ············································································································································ 66
Upgrade of the MLF Control Network System········································································································································· 67

Neutron Science
Neutron Science Section ················································································································································································· 70
BL01: 4D-Space Access Neutron Spectrometer 4SEASONS ················································································································ 72
Oscillating Radial Collimators for the Chopper Spectrometers at MLF in J-PARC ······································································ 74
BL02: Current Status of the Broadband micro-eV Inelastic Neutron Spectrometer DNA ························································ 77
IBRAKI Biological Crystal Diffractometer iBIX··········································································································································· 79
BL04: Developments of New Data Acquisition System and Total Cross-section Measurement Detectors at ANNRI ···· 81
Present Status of BL05 (NOP) ········································································································································································· 84
BL06: Commissioning Status of VIllage of Neutron ResOnance Spin Echo Spectrometers (VIN ROSE)······························ 86
Status Report for BL08 SuperHRPD ····························································································································································· 88
Development of an Advanced Special Neutron Powder Diffractometer under Extreme Environment for Materials··· 90
BL10: NOBORU ···································································································································································································· 92
BL11: Structure Analysis of Crystals and Amorphous Solids at 18 GPa with Paris-Edinburgh Press ···································· 93
High Resolution Chopper Spectrometer at BL12 ··································································································································· 95
BL14 AMATERAS ································································································································································································· 97
Upgrading of TAIKAN ························································································································································································ 99
Development of Elliptic Focusing Mirror for Sample-focusing Neutron Reflectometry at BL16 ·········································· 100
BL17: Neutron Reflectometer SHARAKU ··················································································································································· 102
BL18: Current Status of SENJU ······································································································································································· 104
Status of TAKUMI (BL19)··················································································································································································· 106
The Current Status of the Versatile Neutron Diffractometer, iMATERIA ························································································· 107
Status of the High Intensity Total Diffractometer (BL21, NOVA) ······································································································· 109
Current Status of the Energy-Resolved Neutron Imaging System “RADEN” ················································································· 111
BL23 Polarized Neutron Scattering Spectrometer POLANO ·············································································································· 113
Status of the Common Technical Development ····································································································································· 115
Development of an in-situ SEOP 3He Neutron Spin Filter···················································································································· 116
Sample Environment at MLF ·········································································································································································· 119
Present Status of the MLF Experimental Database ································································································································ 121
Supermirror Coating for Special Figuring ················································································································································· 123
Large Area One-dimensional Scintillator Neutron Detectors for TAKUMI at BL19 ····································································· 124
Development of Alternatives to the 3He Gas-based Neutron Detectors in Nuclear Security················································· 125

Muon Scinece
Status of J-PARC MUSE ····················································································································································································· 128
Installation and Operation of the Muon Rotating Target ···················································································································· 130
Present Status of the D-Line ··········································································································································································· 132
U-Line; Lyman-α Laser Developments and Slow Muon Beamline Commissioning··································································· 134
Construction of the Muon S-Line and Installation of the General Purpose μSR Spectrometer············································· 136
Present Status of the H-Line ··········································································································································································· 138

MLF Safety
Research Safety ··································································································································································································· 142

MLF Operations in 2014
CROSS-Tokai 2014 Update ·············································································································································································· 146
Beam Operation Status at MLF······································································································································································ 151
Users at the MLF ································································································································································································· 152
MLF Proposals Summary – FY2014 ······························································································································································ 153
MLF Division Staff 2014···················································································································································································· 155
CROSS-Tokai Staff 2014 ···················································································································································································· 158
Proposals Review System, Committees and Meetings ························································································································· 160
Workshops, Conferences, Seminars and Schools in 2014 ··················································································································· 166
Award List ············································································································································································································· 169
MLF Publication 2014 ······················································································································································································· 170
Editorial Board - MLF Annual Report 2014················································································································································ 181

Organization Chart

MLF Annual Report 2014

Organization Chart
Organization Chart of
J-PARC Center
Director, J-PARC Center

Organization Chart ofCROSS

Deputy Director (JAEA, KEK, Safety)

CROSS is “Registered Institution for facility Use
Promotion” for the public-access neutron
beam facilities at J-PARC.

Safety Division

President
CROSS Head Office

Accelerator Division

Materials & Life Science Division
Neutron Source Section

Research center for
Science and Society

Director,
CROSS-Tokai
Science Coordinators

Neutron Science Section
Neutron Instrumentation
Section

Safety Division
Administration Division

Muon Science Section
Technology Development
SectionUtilization Promotion
Division
Neutron R&D Division

Particle & Nuclear Physics Division
Transmutation Section

The Role of CROSS-Tokai
Cryogenics Section
Operations Support Section
Information System Section
Public Relations Section
Administration Division
Users Office

Under the terms of the legislation that supports the
Public Neutron Beam Facility, CROSS-Tokai is entrusted with specific responsibilities. In practical terms, thecore functions of CROSS-Tokai can be summarized asfollows:• Proposal Selection and Beamtime Allocation on the
Public Beamlines• User Support on the Public Beamlines• Establishment of an Information Resource for Facility
Users• Outreach and Facility Utilization Promotion• Contract Beamline Assessment and Selection

MLF Annual Report 2014

J-PARC Map
CROSS – Tokai(Ibaraki Quantum Beam Research Center)

J-PARC Center Users Oĸce

R245

(

KEK Tokai㻌 Campus

Main Gate
R245

Linac

HENDEL R&D Building

3 GeV Synchrotron

MLF
50 GeV Synchrotron

J-PARC Map

1m

MLF Annual Report 2014

400ｍm

25 m

BL22 RADEN

Muon and Neutron Instruments

Research and Development
Highlights

Research and Development Highlights

MLF Annual Report 2014

Site Occupancy of Interstitial Deuterium Atoms in FaceCentered Cubic Iron
1. Introduction
The iron (Fe) – hydrogen (H) system has attracted
interest from both scientific and technological point ofview. The H concentration and occupancy in Fe metal lattice provides important information concerning someproperties of the Fe–H system, such as phase stability.
At ambient conditions, a relatively small number of H
atoms dissolve in Fe metal, while under high H2 pressure above several GPa, a hydride, FeHx, is formed. The
in-situ X-ray diffraction measurements were employed
to investigate the hydrogenation process of Fe underhigh H2 pressure and high temperature. The phase diagram of the Fe–H system is established at temperatures
up to 2000 K and pressures up to 20 GPa [1, 2]. In thoseconditions three different phases are exhibited: bodycentered cubic (bcc), double hexagonal close-packed(dhcp), and face-centered cubic (fcc). The fcc-FeHx appeared as a high temperature phase and the H concentration x was estimated to be in the range from 0 to 1.
In the fcc metal lattice there are two interstitial sites capable of accommodating H atoms: octahedral (O) andtetrahedral (T). In the fcc Fe metal, it is considered that
dissolved H atoms would most likely occupy the O siterather than the T site, like in the case of other fcc transition metal hydrides [3]. However, the H occupation sites
and occupancies of the fcc-FeHx still remain unknown.
Because the fcc-FeHx is thermodynamically stable only
under high H2 pressure and high temperature, the attempts to quench it at ambient pressure so far have notbeen successful. Therefore it has been quite difficult todetermine the H occupation states experimentally at
the above mentioned high pressure and high temperature conditions. In this study, we have investigated thedeuterium (D)-occupation state of fcc iron deuteride(FeDx) using in-situ neutron diffraction measurement.
2. Experimental
The in-situ neutron diffraction experiment at highpressure up to about 7 GPa and high temperature below 1000 K was performed using the high pressure neutron diffractometer (PLANET) [4]. The PLANET enables
us to perform in-situ neutron diffraction experiments
at high pressure and high temperature conditions. The
most important feature of PLANET is that it has a 6-axis
multi-anvil press (ATSUHIME) that is good at generating condition of simultaneous high pressure and high2

temperature. A high pressure cell for the in-situ neutron
diffraction was designed based on that for the in-situ
X-ray diffraction [5]. We used an Fe rod with 3 mmϕ ×
2.5 mm in size for the measurement sample. The Fe rod
was placed at the center of a deuterium-sealing capsulemade of NaCl with internal D2 sources of AlD3 pellets
above and below. The NaCl capsule was in a cylindricalgraphite heater embedded in a pressure-transmitting
medium made of ZrO2 (17 mm-edge cube). The highpressure cell was compressed at room temperature up
to 7.4 GPa and then heated to 988 K at a rate of about
40 K per min.
The neutron diffraction profile at 988 K and 6.3 GPafor the structural refinement of fcc-FeDx was accumulated for about 1 hour. We refined the structural parameters
by Rietveld analysis using the Z-Rietveld software (version 0.9.42.2) [6] and succeeded in determining the site
occupancies of dissolved D atoms in the fcc-Fe lattice.
3. Results and discussion
Figure 1 shows the results of the Rietveld refinements of the neutron diffraction profile for the FeDx at
6.3 GPa and 988 K. We first analyzed the results by using the conventional structural model, which is the fcc
structure with D atoms only at O sites (Fig. 2(a)). The
profile seems to be reproduced by this model (Fig. 1(a)).
However, we found a misfit for the 220 reflection peak(inset of Fig. 1(a)). We reconsidered the structural model; based on the structure factor of the fcc-FeDx, the Tsite occupation of the D atom provided additional intensity to the h + k + l = 4m reflection peaks.
Using the new model with the D atoms occupying
both the O and T sites (Fig. 2(b)), the profile was well reproduced and the refined occupancies of the O and T
sites were determined to be 0.532(9) and 0.056(5), respectively (Fig. 1(b)). This unexpected occupation of theD atoms was interpreted in terms of thermally activatedmovement of D atoms by quantum mechanical calculations. Assuming the Boltzmann distribution, the site
occupancy ratio obtained at 988 K yielded an energy
difference between the two sites of 0.19 eV, which wasin agreement with the calculated value of 0.22 eV.
Furthermore, the obtained in situ neutron diffraction data provide a volume expansion rate of the fcc-Fe
due to dissolved D atoms. The volume expansion rate at
6.3 GPa and 988 K can be estimated to be 2.21(4) Å3 per

MLF Annual Report 2014

Research and Development Highlights

Figure 1. Results of Rietveld refinements for diffraction profiles of fcc-FeDx at 988 K and 6.3 GPa. gD(O) and gD(T) stand forthe site occupancies of the O and T sites, respectively. Reliable values for the parameters Rwp and χ2 are given in
the panels. Inset for each panel shows the magnification of diffraction profile around 220 reflection.

Figure 2. Structural models of the fcc-FeDx. The D atoms are accommodated in (a) the only O site and (b) both the O andT sites. Frames colored in red show typical T and O sites.

D atom, which is larger than the value of 1.9 Å3 per D
atom conventionally used for the fcc-FeHx. The volume
expansion rate for the T site occupation is larger thanthat for the O site occupation, hence the larger volume
expansion rate would be interpreted in terms of theslight T site occupation.
References[1] Y. Fukai, Nature 308 (1984) 174.

[2] K. Sakamaki et al., Phys. Earth Planet In. 174 (2009)192.
[3] Y. Fukai, The Metal–Hydrogen System 2nd ed.
(Springer-Verlag, 2005).
[4] T. Hattori et al., Nucl. Instrum. Methods Phys. Res.,
Sect. A 780 (2015) 55.
[5] A. Machida et al., Nat. Commun. 5 (2014) 5063.
[6] R. Oishi et al., Nucl. Instrum. Methods Phys. Res.
Sect. A 600 (2009) 94.

A. Machida1, H. Saitoh1, H. Sugimoto2, T. Hattori3, A. Sano-Furukawa3, N. Endo1, Y. Katayama1, R. Iizuka4, T. Sato5, M. Matsuo5,
S. Orimo5,6, and K. Aoki5
1
Quantum Beam Science Center, JAEA; 2Department of Physics, Chuo University; 3Neutron Science Section, Materials and Life Science
Division, J-PARC Center; 4Geodynamics Research Center, Ehime University; 5Institute for Materials Research, Tohoku University; 6WPIAdvanced Institute for Materials Research, Tohoku University

3

Research and Development Highlights

MLF Annual Report 2014

Simultaneous Characterization of Small-Angle Neutron
Scattering and Bragg-Edge Transmission in Steel

2. Experimental
The chosen steel samples containing Cu and vanadium carbide (VC), which are known as typical precipitates in steels. To form nano-sized precipitates, thesteels were aged at 823 K. The matrices were ferrite in
the Cu steel and partially pearlite in the VC steel.
The SANS experiments were conducted using thetime-of-flight (TOF) SANS instrument BL15 TAIKAN [2].
Each sample was cut into a plate with thickness ofabout 1 mm. To separate nuclear and magnetic scattering contributions, a magnetic field of 1 T was applied tothe samples perpendicular to the incident neutron. In
this condition, since the magnetization is saturated, thescattering profiles parallel to the magnetic field (//H)
contain only the nuclear scattering contribution, whereas the scattering profiles perpendicular to the magnetic
field (⊥H) are composed of both the nuclear and magnetic scattering contributions. The scattering intensities were converted into absolute units using the glasscarbon standard [3]. The neutron transmission spectra
were converted into attenuation coefficient spectra4

to normalize the sample volumes. For the Bragg-edgetransmission analysis, incident neutrons with wavelength between 0.2 and 0.4 nm were used, while thescattering intensity between 0.45 and 0.76 nm was analyzed for SANS. To avoid a possible multiple Bragg scattering, SANS intensity with wavelength below 0.45 nm
was not used.
3. Results and discussion
Figure 1 shows the SANS profiles of the Cu and VC
steels. The SANS profiles of the Cu steel have a shoulder
at q < 1 nm-1, where q is the modulus of the scatteringvector. The shoulder is the onset of the so-called Guinier
region, which reflects the size of scatterers. Hence, theresults indicate that the Cu precipitates are formed in
the Cu steels. The difference in the intensity between//H and ⊥H is attributed to the magnetic scattering
contribution. Since Cu is nonmagnetic, the Cu precipitates have high magnetic scattering contrast with theferromagnetic ferrite matrix.
On the other hand, the VC steel has no shoulder in the SANS profiles. This indicates that almost no
nano-sized precipitates are formed in the VC steels.
Observation conducted with an electron microscope
showed that VC precipitates were not effectively
formed, most likely because cementite consumed carbon. The slope at q < 0.6 nm-1 is probably the scatteringof the large cementite grains.

Cu steel // H
Cu steel ⊥ H
VC steel // H
VC steel ⊥ H

101Intensity (cm-1)

1. Introduction
Steel is one of the most important materials that
support the infrastructure of modern societies. Since
microstructures, such as grain structure, precipitates,and dislocations, play a key role in mechanical properties of steels, the precise characterization of the microstructures in steels is crucial. For example, practicalsteels utilize various strengthening phenomena such as
solid solution hardening, precipitation hardening, work
hardening, and grain refinement. The development ofadvanced steels requires precise control of solvent atoms, precipitates, dislocation, and grain size.
Neutron scattering is a powerful tool to quantitatively characterize the microstructures because neutrons can penetrate thick steel plates and measurelarge sample volumes. In addition, the new-generation
pulsed neutron sources like MLF enable a new characterization technique, i.e., simultaneous analysis of smallangle neutron scattering and Bragg-edge transmission
spectra [1]. This technique provides simultaneously
crystallographic information of the grains from Braggedge and nanostructural information of the precipitatesfrom SANS. In this study, this technique was applied tomodel alloys of precipitation-strengthened steels.

100

10-1

10-2
2

3

4

5 6 7 8 9

10-1

100
q (nm-1)

Figure 1. SANS profiles of Cu and VC steels.

2

MLF Annual Report 2014

{211}

bcc-Fe {110}Attenuation coefficient (cm-1)

2.0

{200}

Figure 2 shows the attenuation coefficient spectra simultaneously measured with SANS. The verticaldotted lines in Figure 2 show the wavelengths of the
Bragg-edges calculated for bcc Fe. A clear jump of theattenuation coefficient is observed at a wavelength ofabout 0.4 nm. This result agrees well with the Braggedge of the bcc Fe {110}. Therefore, we successfullymeasured the SANS and Bragg-edge at the same time

1.5

VC steelCu steel

1.0

0.5
0.2

0.3

0.4

0.5

0.6

0.7

Wavelength (nm)Figure 2. Attenuation coefficient spectra of Cu and VC steels.
Dotted lines indicate the wavelength of Bragg-edges of bcc Fe.

Research and Development Highlights

using TOF-SANS. Small jumps are also found at the
wavelengths of bcc Fe {200} and {211}.
The height of the Bragg-edge is different between
the Cu and VC steels. This indicates the difference in
crystallite size. Since larger crystallite generates higher
multiple Bragg scattering, the height of the Bragg-edge
becomes lower [1,4-6]. Hence, the crystallite size of the
Cu steel is larger than that of the VC steel. Vanadiumprobably delays recrystallization via the solute drag effect in the VC steel.
References[1] Y. Oba, S. Morooka, H. Sato, N. Sato, K. Ohishi, J.
Suzuki, and M. Sugiyama, ISIJ Int. 55, 2618 (2015).
[2] S. Takata, J. Suzuki, T. Shinohara, T. Oku, T. Tominaga,
K. Ohishi, H. Iwase, T. Nakatani, Y. Inamura, T. Ito,
K. Suzuya, K. Aizawa, M. Arai, T. Otomo, and M.
Sugiyama, JPS Conf. Proc. 8, 036020 (2015).
[3] F. Zhang, J. Ilavsky, G. Long, J. Quintana, A. Allen,
and P. Jemian, Metall. Mater. Trans. A 41A, 1151
(2010).
[4] H. Sato, T. Kamiyama, and Y. Kiyanagi, Mater. Trans.
52, 1294 (2011).
[5] T. M. Sabine, Acta Cryst. A44, 368 (1988).
[6] T. M. Sabine, R. B. V. Dreele, and J. E. Jørgensen, Acta
Cryst. A44, 374 (1988).

Y. Oba1, S. Morooka2, H. Sato3, N. Sato1, K. Ohishi4, J. Suzuki4, and M. Sugiyama1
Research Reactor Institute, Kyoto University; 2Department of Aerospace Engineering, Tokyo Metropolitan University; 3Faculty of Engineering,
Hokkaido University; 4Neutron R&D Division, Comprehensive Research Organization for Science and Society

15Research and Development Highlights

MLF Annual Report 2014

Relation between Vickers Hardness and Bragg-edge
Broadening in Quenched Steel Rods
1. Introduction
Bragg-edge transmission imaging is a new material
analysis tool that makes it possible to map non-destructively crystalline microstructural information of bulk
material with spatial resolution around 100 μm over alarge area (about 10 cm × 10 cm) [1]. In this report, we
explain the recent result [2] that indicated the relation
between material hardness and width of d-spacing distribution in a quenched ferritic steel (martensite), obtained by using this method.
Quenching is a popular method to harden steel surface. In the quenched region, martensite is produced,
which has fine microstructure due to carbon solid solution in the crystal structure. We conducted experiments
in order to visualize the quenched region in the thicksteel rods. Real-space distributions of d-spacing (macrostrain) in quenched ferritic steel rods (Fe-0.45%C;
2.6 cm diameter and 2 cm height) were evaluated [3, 4]
by mapping the areas of larger d-spacing of martensite,and successfully identified the quenched spaces as alonger d-spacing area.
However, the deduced {110} d-spacing (0.2042 nm)
in the quenched region was much larger than the normal value (0.2032 nm) of martensite with a compositionof Fe-0.45%C. Furthermore, the Bragg-edge is gentler
in the quenched region than in the ferrite region. To
obtain more accurate evaluation and avoid overestimation, the Bragg-edge broadening caused by microstrain
and crystallite-size effects due to fine microstructureof martensite, which is equivalent to diffraction peakbroadening, should be considered in the analysis.
Thus, a single-Bragg-edge analysis function of the
RITS code [1, 3] was revised so that the Bragg-edge
broadening was reflected in the analysis, then we extracted the information about the width of the d-spacing
distribution. Furthermore, the Bragg-edge width wascompared with the Vickers hardness in ferrite and martensite, and it was indicated that the width is proportional to the Vickers hardness. The result suggests thatthe Bragg-edge transmission imaging can be used as a
non-destructive method to investigate quenched steels.
2. Development of the Bragg-edge broadening
analysis method
For d-spacing/macrostrain analysis, the profile fitting analysis method was used. In the RITS code, the6Jorgensen-type edge-profile function was adopted [3].
This function is derived from the convolution of the
Heaviside step function and a Gaussian function withtwo back-to-back exponentials.
So far, the edge-profile function was constant andindependent of the pixel position. This is because theinstrumental resolution, which is expressed by the
Jorgensen-type edge-profile function, is usually notchanged. Therefore, the analysis is correct if the shapeof d-spacing distribution remains the same. However,for a ferritic steel containing martensite, the distribution of d-spacing changes with the content of martensite. The width of d-spacing distribution (the Bragg-edge
broadening) of martensite is larger than that of ferrite.
In other words, for analysis of a ferritic steel containing martensite, another broadening parameter for thisphenomenon should be implemented into the edgeprofile function.
In the new analysis procedure, it is assumed thatthe distribution of d-spacing depending on microstrain
and crystallite-size follows a Gaussian function. Then,the whole Jorgensen-type edge-profile function consists of two functions. One is the Jorgensen-type instrumental resolution function, and the other is theGaussian d-spacing distribution function. In the actual
analysis, firstly, we analyze the sharp Bragg-edge dataof the region which consists mainly of ferrite to determine the Jorgensen-type instrumental resolution function. Secondly, we evaluate the average (macrostrain)
and the width (microstrain) of the Gaussian d-spacing
distribution function by using the Jorgensen-type instrumental resolution function obtained in the firststage analysis.
3. Experimental
The specimens were three sections of ferritic steelrod (Fe-0.45%C; 2.6 cm diameter and 2 cm height)
quenched from each rim surface by axial-symmetricinduction hardening. The quenched depth from thesurface was expected to be 3 mm, 5 mm and 7 mm, respectively. Neutrons were transmitted along the axial
direction of the sample cylinder (2 cm thickness).
The pulsed neutron transmission imaging experiment was carried out at J-PARC MLF BL10 “NOBORU” [5].
The beam angular divergence was ± 3 mrad in this experiment. The neutron TOF imaging detector used wasMLF Annual Report 2014a neutron 10B-MCP (Micro Channel Plate) detector [6].
The pixel size was 55 μm, and the detection area was
1.4 cm × 1.4 cm.
4. Results and discussion
Fig. 1 shows Bragg-edge transmission spectra of thecenter (ferrite) region and the rim (martensite) region of
the 7 mm-depth quenched rod. This figure shows thatboth {110} Bragg-edge data can be reproduced by thedeveloped data analysis procedure. Additionally, it was
found that the extracted d-spacings were reasonable(0.2026 nm for ferrite and 0.2032 nm for martensite). An
overestimation on d-spacing of martensite (0.2042 nm),
evaluated in the previous work [3, 4], was corrected bythis analysis method. Furthermore, an FWHM of theGaussian d-spacing distribution due to microstrain andcrystallite-size was estimated in a value of the order of
10−3 nm from the data in the martensite region.
Fig. 2 shows results of the FWHM mapping of
the d-spacing distribution of 7 mm, 5 mm and 3 mm
quenched steel rods. It is clear from the first sight at the

Neutron transmission

35%

Center (ferrite)d = 0.2026 nm
w = 2.0 × 10-4 nm

30%
25%

Rim (martensite)20%

d = 0.2032 nm
w = 5.4 × 10-3 nm

Center (exper.)Center (fit.)
Rim (exper.)Rim (fit.)

15%
10%
5%
0%
0.395

0.405

0.415

0.425

Neutron wavelength / nm
Figure 1. {110} Bragg-edge transmission spectra with the fitting curves of ferrite (center) region and martensite(rim) region in the 7 mm-depth quenched rod.

Research and Development Highlights

images that the areas with value of the order of 10−3nm almost correspond to the expected quenched area
depth (7 mm, 5 mm or 3 mm) from the rim surface.
The significance of the obtained parameter is discussed in terms of the quantity of martensite by using
the Vickers hardness data. At first, we calculated the radially dependent data of the width of d110-spacing, w110,
of each rod from Fig. 2. Figure 3 (a) shows radial changes of w110 of 7 mm-, 5 mm- and 3 mm-depth quenchedrods. Continuously, we fitted the sigmoid functions to
the radial dependences (curves in Fig. 3 (a)), and derived the inflection point of each curve (vertical dashedlines in Fig. 3 (a)). As a result, the inflection points are
6.5 mm, 5.2 mm and 3.3 mm for 7, 5 and 3 mm-depth
quenched rods. These seem to correspond to the actual
depths of quenching.
To verify this estimation, Fig. 3 (a) was comparedwith the radial dependence of the Vickers hardness,
which correlates to the ratio of ferrite/martensite. In
particular, the Vickers hardness of 450 (Hv 450) is wellknown as the hardness boundary between ferrite andmartensite. Figure 3 (b) shows the radial dependence of
the Vickers hardness of each quenched rod. From thisfigure, it was found that the shape of radial dependenceof w110 was quite close to those of the Vickers hardness for each quenched rod. Additionally, the points of
Hv 450 also correspond to the inflection points of radial
dependence of w110. Therefore, these results indicatethat w110 depicts the ferrite/martensite concentration
ratio in a ferritic steel.
Finally, we deduced the relation between the
Vickers hardness and w110 by comparing both values atthe same position. Figure 4 shows plots of the Vickers
hardness as a function of w110, with the fitting lines. This
figure shows that the Vickers hardness and the ferrite/
martensite quantity are proportional to w110.

(a) 7 mm depth quenched rods
FWHM of d110-spacing distribution
(nm)
0.005

(b) 5 mm depth quenched rods
FWHM of d110-spacing distribution
(nm)
0.005

(c) 3 mm depth quenched rods
FWHM of d110-spacing distribution
(nm)
0.005

0.004

0.004

0.004

0.003

0.003

0.003

0.002

0.002

0.002

0.001

0.001

0.001

0.000

0.000
5 mm

5 mm

0.000
5 mm

Figure 2. Real-space map (55 μm pixel size) of FWHM of the d-spacing distribution in quenched steel rods. The quenched (martensite) regions exist near the rim surface.

7

Research and Development Highlights

MLF Annual Report 2014(a) Radial dependence of w110(b) Radial dependence of Vickers hardness

Distance from the rim / mm
10

8

6

6.5

0.004

5.2

4

Distance from the rim / mm
2

3.3

0

10

8

800

5 mm

0.003

w110 / nm

12

7 mm

0.002
0.001
3 mm

Vickers hardness

12

6.5

6

4

5.2

2

3.3

0

Martensite

600
Hv 450400

7 mm
Ferrite

200

3 mm

5 mm

0

0.000
0

2

4

6

8

10

12

Distance from the center / mm

0

2

4

6

8

10

12

Distance from the center / mmFigure 3. (a) Radial dependences of FWHM of d110-spacing distribution, and (b) radial dependences of the Vickers hardness, of
7 mm-, 5 mm- and 3 mm-depth quenched steel rods.

Vickers hardness

800
700
600

using this method. Furthermore, it is expected that the
information about dislocation density and crystallite
size can be evaluated by further improvement of the
Bragg-edge profile analysis.

Hv7mm = 210927w110,7mm + 23.051
Hv5mm = 188980w110,5mm + 109.09
Hv3mm = 198199w110,3mm + 50.372

500
400
7 mm
5 mm
3 mm

300
200
100
0.00040.00140.00240.0034w110 / nm
Figure 4. Relation between the Vickers hardness and FWHM
of d110-spacing distribution in quenched steel rods.

5. Conclusion
By using the pulsed neutron transmission imaging
combined with the revised RITS code, the Bragg-edge
broadening due to martensite in a bulk ferritic steel was
analyzed over a large area with high spatial resolution.
As a result, the width of d-spacing distribution related
to hardness, ferrite/martensite quantity, microstrain
and crystallite-size could be successfully evaluated.
Furthermore, it was found that the Vickers hardness
was linearly proportional to the width of d-spacing
distribution.
The use of this method is viable because it is nondestructive. The condition for this is that the width
should not depend on the measuring direction, namely
the scalar value. It is expected to be scalar since themartensite texture is not strong. Therefore, in the future,
non-destructive measurements of the material hardness in a ferrite/martensite steel may be carried out by

Acknowledgments
The authors are greatly thankful to Dr. Anton S.
Tremsin of University of California at Berkeley for using
the MCP detector, and the NOBORU instrument scientists for their experimental assistance. This work was
supported by Grant-in-Aid for Scientific Research (S)No. 23226018 from JSPS.
References[1] H. Sato, T. Kamiyama and Y. Kiyanagi, Mater. Trans.
52, 1294-1302 (2011).
[2] H. Sato, T. Sato, Y. Shiota, T. Kamiyama, A. S. Tremsin,
M. Ohnuma and Y. Kiyanagi, Mater. Trans. 56, 11471152 (2015).
[3] Y. Kiyanagi, H. Sato, T. Kamiyama and T. Shinohara, J.
Phys. Conf. Ser. 340, 012010 (2012).
[4] T. Kamiyama, H. Sato, R. Takamori, N. Ayukawa, Y.
Iwasaki, A. S. Tremsin and Y. Kiyanagi, MLF Annual
Report 2010, 115-117 (2011).
[5] F. Maekawa, K. Oikawa, M. Harada, T. Kai, S. Meigo,
Y. Kasugai, M. Ooi, K. Sakai, M. Teshigawara, S.
Hasegawa, Y. Ikeda and N. Watanabe, Nucl. Instrum.
Methods A 600, 335-337 (2009).
[6] A. S. Tremsin, J. B. McPhate, A. Steuwer, W.
Kockelmann, A. M. Paradowska, J. F. Kelleher, J. V.
Vallerga, O. H. W. Siegmund and W. B. Feller, Strain
48, 296-305 (2012).

H. Sato1, T. Sato1,2, Y. Shiota1,3, T. Kamiyama1, M. Ohnuma1, and Y. Kiyanagi1,3
Graduate School of Engineering, Hokkaido University; 2Present afﬁliation: Muroran Plant, The Japan Steel Works, Ltd.; 3Present afﬁliation:
Graduate School of Engineering, Nagoya University

1

8

MLF Annual Report 2014

Research and Development Highlights

Study of the Structural Change in the Human Stratum
Corneum Induced by the Treatment of Surfactant Solutions
1. Introduction
The outermost layer of the skin, stratum corneum(SC), consists of corneocytes and intercellular lipid matrix, as shown schematically in Figure 1. The structureof the SC plays an important role in the barrier function [1, 2]. The surfactant used in skin cleansers sometimes induces swellings of SC. They are accompanied bystructural changes in the keratin fibers in the corneocytes, as well as in the intercellular lipids lamellar structure around the corneocytes. The aim of this research is
to study the conformation change of human SC, particularly the soft keratin conformation, induced by the treatment of surfactant solutions using scattering analysis.
A problem emerged while conducting small-angle
X-ray scattering (SAXS) measurements – the scatteringof the surfactant micelles disturbed the observation of
keratin fibers, particularly microfibril structures. To resolve this problem, the influence of the scattering of
surfactant micelles was eliminated by using deuterated
surfactant solutions in the small-angle neutron scattering (SANS) measurements, and observing only keratin
fibers in the heel SC powder (without the intercellularlipids lamellar structures) became possible [3]. Using
this technique, this year, we analyzed the swelling of
the keratin fiber in SC powder soaked with the surfactant solution of various conditions.
On the other hand, since the SANS measurement
required long time, several hours per one scan, it wasdifficult to pursue SC structural change in a short time(from several minutes to 1 hour) after surfactant solution soak. Therefore, the SC internal structure change
was measured by SAXS for a short time using the structural orientation in the stacked SC sheets. And the SAXS
measurement results after prolonged progress werecompared with the SANS measurement results.
2. Experimental
The SANS experiments were performed using the
TAIKAN instrument installed on the BL15 beamline at
the MLF, J-PARC (Tokai, Japan). The SAXS experiments
were performed using the SAXS spectrometer installedon the BL19B2 beamline at the SPring-8 (Sayo, Japan).
The human heel SC powder was obtained from thehealthy volunteer from Kao Corporation. We confirmedthat the powder samples had no peaks of the intercellular lipids lamellar structure by SAXS and WAXS. The

human abdominal SC sheets were supplied by Biopredic
International (Rennes, France). As a surfactant solution
for soaking, the 3% and pH 7 sodium dodecyl sulfate(SDS) solution was prepared. Deuterated SDS (d-SDS)
solution in heavy water and heavy water were used for
the SANS experiments instead of the usual SDS solution
and water, respectively.
The SANS experiments were conducted at 30, 40, or
50°C using the heater of the automatic sample changer.
All SAXS experiments were conducted at RT (26-27°C)
without the heater.
Corneocytes and lipid matrixes

SC
20μm

Lipid
Lipid matrix
matrixKeratinKeratin fibers
fibersOne
One corneocyte
corneocyte

Inside of corneocyte
Figure 1. Schematic diagram of the stratum corneum (SC)structure.

3. Results and discussions
Figure 2 shows the result of the SANS measurements of SC powder soaked with the d-SDS solution
or the heavy water. The contrast-matching techniqueusing deuterated surfactant solutions enabled comparison of the swelling of keratin fibers. The peak position shifted toward lower q and the peak width became
broader, by soak of d-SDS solution than heavy water.
Furthermore, systematic peak shift toward a lower q
and broadening took place by increasing the temperature. These were considered to be the results in which
the keratin fiber swelled more.
Figure 3 shows the results of SAXS and SANS measurements of SC sheets. We analyzed the scatteringprofiles of the vertical and parallel direction separately
since the scattering profiles of measurements using thestacked SC sheets have anisotropy. Since the keratin
9Research and Development Highlights

Intensity (cm-1)(a)

MLF Annual Report 2014

SPring-8䟺SAXS䟻

103

J-PARC/MLF䟺SANS䟻SC (powder) + 3% d-SDS/D2O
50䉔
40䉔
30䉔

102

㼓㼄㼕㼄㼏㼏㼈㼏
101

100

10-1 6 8
10-1

Intensity (cm-1)

(b)

2

4

6 8

2

4

100
q (nm-1)

6 8

2

101

103
SC (powder) + D2O
50䉔
䚭䚭
40䉔
䚭䚭
30䉔
䚭䚭

102

㼓㼄㼕㼄㼏㼏㼈㼏

101

100

10-1 6 8
10-1

2

4

6 8

2

100
q (nm-1)

4

6 8

2

101

Figure 2. SANS profiles of SC powder soakedwith (a) surfactant solutions (SC + 3%
d-SDS/D2O) and (b) heavy water (SC +D2O) at pH 7. Arrows indicate the 1st
interference peak position of spacingof swollen keratin fibers at 50°C.

Figure 3. SAXS (a,b) and SANS (c,d) profiles of stacked SC sheets. (a,c)
soaked with surfactant solutions, (b,d) soaked with (heavy) water.
Blue filled-in arrows indicate the 1st interference peak position of
spacing of swollen keratin fibers. Red filled-in arrows indicate thepeak position of the intercellular lipids lamellar structure. Blackoutlined arrows indicate the peak position of the SDS micelles.

fibers and the intercellular lipids lamellar structure exist
in parallel with the SC sheet, their perpendicular scattering peaks became stronger. By comparing the resultsof the SAXS and SANS measurements, a significant difference emerged in the peak of the intercellular lipids
lamellar structure. The peak of the intercellular lipids lamella structure was not so prominent in the SANS measurement. Moreover, the peaks of the intercellular lipids
lamella structure were almost the same after soaking inboth SDS solution and water in the SAXS measurement.
These results suggested that wetting of surface of theskin by the surfactant solution of several percent or thewater did not change intercellular lipids lamella structure
mostly. Furthermore, the SANS result indicated that (deuterated) water outside of the skin did not penetrate thewater layers in the intercellular lipids lamella structure.

It became clear that the keratin fiber swelled more
quickly and largely by soaking the SDS solution rather
than water, according to the short-term SAXS measurement of the SC internal structure change using thestacked SC sheets (data not shown) [4]. Consequently,
the usefulness of the method of analyzing SC structuralchange using the stacked SC sheets was suggested.
References[1] S. H. White et al., Biochemistry 27 (1988) 3725.
[2] J. A. Bouwstra et al., Biochim. Biophys. Acta 1212
(1994) 183.
[3] T. Kume et al., Hamon 24 (2014) 15.
[4] T. Kume et al., SPring-8/SACLA Research Reports Early
edition (2015) 2014A1516.

T. Kume1, M. Onoo1, and I. Hatta2
Analytical Science Research Labs. Kao Corporation; 2Nagoya Industrial Science Research Institute1

10MLF Annual Report 2014

Research and Development Highlights

Understanding the Mechanism of Gene Expression by
Flexibility of the DNA Structure - Observation of Basesequence Dependent DNA Dynamics by Quasi-elastic
Neutron Scattering
1. Introduction
The genomes (DNA sequences) of many organisms
have been obtained, and a research base for analyzing
and predicting the biological function from a genome
has been established. However, during the process ofgene expression, amino acids and bases interact witheach other to form a complex tertiary structure of protein and DNA, and a clear match between gene sequenceand biological function cannot necessarily be seen.
Recent studies have shown that the direct interaction between protein and DNA (known as “direct recognition”) is not the only important factor in passing
the information contained within a genome, but so
is the “indirect recognition,” which is an easy transformation of the sequence-dependent DNA structure(Fig. 1). Because the analysis of the fluctuations in thesequence-dependent DNA structure under indirect
recognition is important, it is necessary to experimentally demonstrate that the dynamics of DNA can be observed directly by experiment [1].

Figure 1. Bending of DNA by protein binding. Dotted line indicates the stable DNA conformation, but the conformation accommodates the bending dependingon base sequence.

2. Results & Discussions
In this study, we performed quasi-elastic neutron
scattering experiments using the AMATERAS instrument at J-PARC/MLF to study the dynamics of two kindsof DNA sequences: 5’CGCGAATTCGCG3’ (AATT) and
5’CGCGTTAACGCG3’ (TTAA). These sequences were predicted to be rigid and flexible, respectively, by analysis
of a systematic molecular dynamics simulation. We successfully acquired neutron spectrum with the required
precision (Fig. 2).

Figure 2. Neutron quasi-elastic scattering spectrum have thesignal which an energy change spread through for
0 elastic scattering symmetrically.

Examining the half-width at half maximum (HWHM)
of the spectrum as a function of Q provides informationon the relaxation time of the DNA dynamics. HWHM increases with Q2 at the lower Q region, and asymptotically approaches a constant value at large Q for bothsequences. The constant value of TTAA was larger thanthat of AATT in the high Q region, although they weresimilar to each other in the low Q region. This indicatesthat the diffusive motion is dominant with similar frequency for both sequences at longer length scales,
whereas at shorter length scales, the frequency of motion of TTAA is larger than that of AATT. The plateau of
HWHM at higher Q region indicates that the correlation
times are independent of the length scale, suggestingthat the jump motion dominates toward smaller lengthscales. These behaviors can be well explained by thejump diffusion model [2], as follows
DQ2
Γ(Q) =
1 + DQ2τ0
The fitting curves to the data are shown in
Fig. 3. The diffusion coefficients, 6.0±0.8 nm2*s−1 and
5.5±0.5 nm2*s−1 for AATT and TTAA, respectively, are thesame within the error range. The residence time of a hydrogen atom on one site is calculated as τ = 1/Γ(Q→∞),
where Γ(Q→∞) is HWHM obtained from the asymptotic
behavior at higher Q. The resulting residence times are
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MLF Annual Report 2014

the recognition of DNA, as has been proposed based on
simulations and statistical analyses of crystal structures.
This result demonstrates that DNA sequences
should include not only the string of bases but also information about the DNA flexibility. We expect that thediscovered structural property of DNA in this study willcontribute to elucidation of the mechanism controllingthe “on–off switch” of gene-expression.

Figure 3. HWHM of QENS spectrum of AATT and TTAA dodecamers.

τ = 45.2±1.5 ps and τ = 40.9±1.1 ps for AATT and TTAA,
respectively. The residence time of AATT is longer thanthat of TTAA.
This result demonstrates agreement with the molecular dynamics simulation [3] and supports the importance of the indirect interaction of DNA flexibility in

3. Acknowledgments
This study was partially subsidized with scientificresearch funds from the Ministry of Education, Culture,
Sports, Science and Technology (No. 18031042).
References[1] H. Nakagawa et al., Phys. Rev. E., 90 022723 (2014).
[2] Y. Yonetani et al., Biophys. Chem. 160 54 (2012).
[3] M. Bee, Quasielastic Neutron Scattering: Principles
and Applications in Solids State Chemistry, Biology
and Materials Science (Adam Hilger, Bristol, UK,1988).

H. Nakagawa1,2, Y. Yonetani1, K. Nakajima2, S. Ohira-Kawamura2, T. Kikuchi2, Y. Inamura2, M. Kataoka3, and H. Kono1
Quentum Beam Science Center, Japan Atomic Energy Agency; 2J-PARC Center, Japan Atomic Energy Agency; 3Graduate School of Materials
Science, Nara Institute of Science and Technolog

1

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MLF Annual Report 2014

Research and Development Highlights

QENS Study of Protein Dynamics in Glycerol and Water
Mixture Measured on DNA
1. Introduction
Protein in solution has a dynamical hierarchy fromdiffusion to structural dynamics (internal motions). The
protein diffusion contributes to the transportation of
the protein as a colloidal particle in solution and subsequently it improves the efficiency of the encounterof an enzyme with substrate. The structural dynamics isclosely related to the protein function, such as the substrate binding of the enzyme. The protein dynamics areaffected by the physicochemical propitiates of the solvent, such as viscosity and solute concentration (crowding). In vivo, the intracellular environment displays highviscosity and it is also crowded. Glycerol is used as a
low-molecular weight-crowding agent. Furthermore,glycerol is accumulated inside the bodies of some insects as bioprotectant [1]. Therefore, it is important toexamine the effect of glycerol on protein dynamics.
In this study, the global diffusion and structuraldynamics of hen egg white lysozyme in glycerol-water
mixtures between 0 and 50% glycerol (v/v) were examined by quasi-elastic neutron scattering experiment at
BL02 in J-PARC/MLF.
2. Results & Discussions
Figure 1 shows the quasi-elastic neutron scattering
spectrum of lysozyme in D2O solution at Q = 0.625 [Å−1].
To characterize the global diffusion and structural dynamics of the protein, the experimental data wereanalyzed by the following function, which includes
the contributions of the global diffusion and internalmotions,

Figure 1. Quasi-elastic neutron scattering spectrum of lysozyme in D2O solution at Q = 0.625 [Å–1]. The red
curve is the fitting curve of double Lorentzian.

Sp(Q,ω) = Sdif (Q,ω)⊗Sin(Q,ω)= Ldif (Γdif ,ω)⊗[EISF⋅δ(ω) + (1−EISF)⋅Lin (Γin ,ω)]= [EISF⋅Ldif (Γdif ,ω) + (1−EISF)⋅Ltot (Γtot ,ω)]L(Γ,ω) is a Lorentzian function. And Ltot(Γtot,ω) represents the convolution of global diffusion and internalmotions, where Ltot = Γdif + Γin. The scattering profile wasadequately described by the above fitting function, as
shown in Fig. 1.
Inset of Fig. 2 is the Half-Width at half-Maximum(HWHM = Γdif) of QENS from the global diffusion. The
HWHM is proportional to Q2, and the diffusion constants are obtained by the following equation:
Γ = DQ2
The diffusion constant decreases as the glycerol
concentration increases due to the viscosity.

Figure 2. Protein diffusion constant as a function of glycerol
concentration. The inset shows the HWHM (= Γdif )from protein global diffusion contribution.

Next, in order to examine the internal motions,
EISF were analyzed. EISF data provide information on
the conformational space geometries of protein dynamics. Here, we analyze the EISF with the continuous
diffusion model within a restricted spherical volume(DSV). In DSV model, EISF is described as the following
equation [2]:EISF = p + (1 − p)·[3·J1(qr)/(qr)]2
Here, J1(x) is the first-order Bessel function. The p accounts for the fraction of H atoms that do not undergo
DSV motions on the measured time scale, and r is theradius of a hard-walled restricted sphere. Fig. 3a shows13

Research and Development Highlights

MLF Annual Report 2014

EISF and the fitting curves with the DSV model.
In Fig. 3b, p increases and r decreases as the glycerol concentration increases. These results indicate thatthe protein’s internal motions are slowed down and theamplitude of the structural fluctuations is restricted byglycerol.
In conclusion, glycerol affects both the global diffusions and internal structural motions of protein, andreduces the protein dynamics in both time- and spacescale. This would lead to the reduction of enzymatic
activity in the presence of glycerol. These effects ofglycerol on bio-materials may be related to insects’ resistance to low temperatures.

Figure 3. (a) EISF and fitting curves with the DSV model. (b)Immobile fraction p on the measured time scale,and the radius r of a hard-walled restricted sphere.

References[1] C. Plolge et al., Nature, 164 666 (1949).
[2] M. Bee, Quasielastic Neutron Scattering: Principles
and Applications in Solids State Chemistry, Biology
and Materials Science (Adam Hilger, Bristol, UK,1988).

H. Nakagawa1,2, K. Shibata2, and T. Yamada3
Quentum Beam Science Center, Japan Atomic Energy Agency; 2J-PARC Center, Japan Atomic Energy Agency; 3CROSS-Tokai

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MLF Annual Report 2014

Research and Development Highlights

Neutron Crystallography Reveals Two Protonation
States of PcyA, a Bilin Reductase
1. Introduction
Phycocyanobilin: ferredoxin oxidoreductase (PcyA),
which is a major member of the ferredoxin-dependentbilin reductase (FDBR) family, catalyzes two steps ofthe two-proton-coupled two-electron reduction ofbiliverdin IXα (BV) to phycocyanobilin (PCB), one ofthe phytobilins [1]. Phytobilins, light harvesting andphotoreceptor pigments in higher plants, algae andcyanobacteria, are synthesized from BV by FDBRs. PCB
comprises the chromophore of algal phytochromes
and the core phycobiliprotein antennae of cyanobacteria and red algae.
In the catalysis, PcyA strictly controls the regiospecificity and reaction sequence of the BV reduction;
reduction of the BV D-ring exo-vinyl group to generate
the reaction intermediate, 181,182-dihydrobiliverdin
IXα (18EtBV) precedes the A-ring endo-vinyl reduction.
Moreover, PcyA is unique not only because of its ability
to catalyze the sequential reduction of two vinyl groups,
but also because it is the only enzyme that catalyzes the
BV D-ring reduction among FDBRs (Figure 1) [2].
Several unique features of PcyA catalysis have been
revealed. First, the existence of two types of positively
charged BV (BVH+) states has been proposed when BV
is bound to PcyA. One is an N-protonated structure inwhich four pyrrole N atoms of BV are fully protonatedand the bis-lactam state is preserved [3]. The other isan O-protonated structure in which one or two lactim(C-OH) group(s) is (are) formed [4]. It has been also indicated that His88 and Asp105 are essential residues,

both of which are located near the substrate BV andthought to be proton donors [5-8]. The side chain of
Asp105 showed dual conformations in the structuresof the PcyA-BV and PcyA-18EtBV complexes. It was
proposed that a water molecule (“axial” water) in theactive site, which was ejected upon one electron reduction, was essential for catalysis [4]. A proton-coupledelectron transfer mechanism including the axial watermolecule was proposed for its catalysis. However, this
proposed mechanism has to be reassessed due to two
issues. The first issue is that we could not identify theaxial water molecule in the structure of the previous“cryo” wild-type PcyA-BV complex [6]. The second oneis the uncertainty of the protonation states of the PcyABV complex. Knowing the protonation states of thesubstrate BV and of these essential residues is criticalfor understanding the catalytic mechanism of the PcyA
reaction involving proton transfer.
It is difficult to determine the protonation stateof the PcyA-BV complex. X-rays are known to generate electrons or harmful charged by-products wheninteracting with solvent molecules in protein crystals.
The charged products might cause enzymatic and/or
accidental side reactions and concomitant structuralchanges, thus resulting in incorrect structural information in studies of redox enzymes [9-11]. Furthermore,as some residues, including Asp105, have dual conformations in the PcyA-BV complex [6], the occupancies ofhydrogens on such residues must be lower, making itmuch more difficult to determine their locations.

Figure 1. The PCB biosynthesis catalyzed by PcyA.

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MLF Annual Report 2014

Figure 2. Chemical structures for two protonation states of the PcyA active site and BV (both sides) and the overall structure of thePcyA-BV complex (red; oxygen, green; carbon, blue; nitrogens).

To understand the unique reaction mechanism of
PcyA, we used neutron crystallography to determine thestructure of PcyA from Synechocystis sp. PCC 6803 complexed with BV, revealing the exact location of the hydrogen atoms involved in the catalytic reaction of PcyA [12].
2. Results and Discussions
This was the first study of the neutron structure ofa FDBR family member that revealed the protonation
state of BV and the surrounding residues. The resolution was 1.95 Å, and 1.50 Å resolution of the neutron
and X-ray data, respectively [12]. Notably, approximately half of the BV bound to PcyA was BVH+, a statein which all four pyrrole nitrogen atoms were protonated. The protonation states of BV (neutral BV and BVH+)
were in concert with the protonation of the adjacent
Asp105, and two Asp105 conformations were involvedin the catalytic activity of PcyA. Protonated Asp105
formed hydrogen bonds with both lactam oxygen andpyrrole nitrogen atoms in the D-pyrrole ring, whereas
deprotonated Asp105 formed hydrogen bonds withthe pyrrole nitrogen atoms of the B- and D-pyrrole rings(Figure 2). We also succeeded in identifying the “axial”
water molecule that interacts with the neutral pyrrole
nitrogen of the A-ring, which is believed to be essential
for the A-ring reduction. The elucidated protonation
states of the substrate BV and the surrounding residues
determined by the present neutron crystallography imply that Asp105 and the axial water molecule are likely
to contribute to the proton transfer in PcyA catalysis.
Additionally, we found a hydronium ion between theessential His88 and the nearby His74. This hydronium
ion is also likely to facilitate proton-transfer to the activesite. This discovery of a hydronium ion in protein structure was the third such case worldwide [13, 14].
16

3. Acknowledgment
We thank the members of IBARAKI Biological
Crystal Diffractometer in J-PARC for the neutron diffraction data collection. The neutron diffraction experiment
was conducted under proposal 2012PX0011 (Ibaraki
Prefecture Project). We thank Dr. Yusuke Yamada andthe other members of the Structural Biology beamlinesof PF and members of BL41XU of SPring-8 for X-ray diffraction data collection, including the preliminary experiments. The X-ray diffraction experiments in PF wereconducted under proposals 2011G519 and 2013G504.
Crystallization under microgravity was attempted in
the “Kibo” project of the Japan Aerospace Exploration
Agency (JAXA). We are grateful to Professor Takamitsu
Kohzuma of Ibaraki University for his support and fruitful discussion regarding crystallization. We also thankProfessor Masao Ikeda-Saito’s laboratory at Tohoku
University for use of the microspectrophotometer. This
work was partly supported by JSPS KAKENHIs numbers
24570122, 22770096 (to M.U.) and 23370052 (to K.F.,
K.W., and M.U.).
References[1] N. Frankenberg, J. C. Lagarias, J. Biol. Chem., 278,
9219-9226 (2003).
[2] M. Unno, M. Sugishima, K. Wada, K. Fukuyama,
Integrating Approach Photofunctional Hybrid
Materials for Energy and the Environment, Akitsu,
T. (ed), Nova Publishers, N.Y., 47-67 (2013).
[3] S. L. Tu, A. Gunn, M. D. Toney, R. D. Britt, J. C. Lagarias,
J. Am. Chem. Soc. 126, 8682-8693 (2004).
[4] A. C. Kohler, D. D. Gae, M. A. Richley, S. Stoll, A.
Gunn, S. Lim, S. S. Martin, T. I. Doukov, R. D. Britt, J. B.
Ames, J. C. Lagarias, A. J. Fisher, A. J., Biochemistry,49, 6206-6218 (2010).

MLF Annual Report 2014[5] Y. Hagiwara, M. Sugishima, H. Khawn, H. Kinoshita,
K. Inomata, L. Shang, J. C. Lagarias, Y. Takahashi, K.
Fukuyama, J. Biol. Chem., 285, 1000-1007 (2010).
[6] Y. Hagiwara, M. Sugishima, Y. Takahashi, K.
Fukuyama, Proc. Natl. Ac. Sci. U.S.A., 103, 27-32(2006).
[7] Y. Hagiwara, M. Sugishima, Y. Takahashi, K.
Fukuyama, FEBS lett. 580, 3823-3828 (2006).
[8] S. L. Tu, W. Sughrue, R. D. Britt, J. C. Lagarias, J. Biol.
Chem., 281, 3127-3136 (2006).
[9] B. Chance, P. Angiolillo, E. K. Yang, L. Powers, FEBS
lett. 112, 178-182 (1980).
[10] G. I. Berglund, G. H. Carlsson, A. T. Smith, H. Szoke,

Research and Development Highlights

A. Henriksen, J. Hajdu, Nature 417, 463-468 (2002).
[11] J. Wuerges, J. W. Lee, Y. I. Yim, H. S. Yim, S. O. Kang,
K. Djinovic Carugo, Proc. Natl. Ac. Sci. U. S. Am. 101,
8569-8574 (2004).
[12] M. Unno et al., J. Am. Chem. Soc. 137, 5452-5460(2015).
[13] M. G. Cuypers, S. A. Mason, M. P. Blakeley, E. P.
Mitchell, M. Haertlein, V. T. Forsyth, Angew. Chem.
Int. Ed. Engl. 52, 1022-1025 (2013).
[14] A. Y. Kovalevsky, B. L. Hanson, S. A. Mason, T.
Yoshida, S. Z. Fisher, M. Mustyakimov, V. T. Forsyth,
M. P. Blakeley, D. A. Keen, P. Langan, Angew. Chem.
Int. Ed. Engl. 50, 7520-7523 (2011).

M. Unno1,2, K. Ishikawa-Suto1,2,3, K. Kusaka2, T. Tamada3, Y. Hagiwara4, M. Sugishima5, K. Wada6, M. Ishihara2, and K. Fukuyama7
Graduate School of Science and Engineering, Ibaraki University; 2Frontier Research Center for Applied Atomic Sciences, Ibaraki University;
3Quantum Beam Science Center, Japan Atomic Energy Agency; 4Department of Biochemistry and Applied Chemistry, Kurume National College
of Technology; 5Department of Medical Biochemistry, Kurume University School of Medicine; 6Organization for Promotion of Tenure Track,
University of Miyazaki; 7Graduate School of Engineering, Osaka University

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MLF Annual Report 2014

Phonon Anomaly in La1.5Sr0.5NiO4
1. Introduction
La2−xSrxNiO4 is isostructural to one of the typicalcuprate superconductors La2−xSrxCuO4. Similarly to thecuprates, one hole per Ni ion is introduced in the NiO2
planes by the substitution of a La3+ ion with a Sr2+ ion. In
the course of exploring the origin of the superconductivity in cuprates, the role of phonons has been extensively studied, and it was revealed that the hole doping
induces a strong anomaly in the Cu-O bond stretchingmode [1]. The phonon anomaly was seen as a result of
the electron-lattice coupling associated with charge inhomogeneity in the CuO2 planes [2]. In the nickelates,
the electron-lattice coupling is considered to be larger
than in the cuprates, as the charge inhomogeneity appears in the more obvious form of static charge stripes
along the direction diagonal to the Ni square lattice.
Then, phonons in the nickelates have been studied byinelastic neutron scattering (INS) to investigate whether the doped holes or charge stripes affect particularly
the bond-stretching modes, which are the highest-energy longitudinal optical (LO) modes in this system. It
was revealed that the LO modes are susceptible to thenon-stoichiometry [3, 4] and hole-doping [5, 6], showing similar softening as in cuprates, but the anomalies
in the phonons are independent of the charge stripe
wave vector [6].
In the present study, we performed an INS studyof the high-energy phonons in a single crystal of
La1.5Sr0.5NiO4 [7]. In this composition, the charge ordering results in a nearly checkerboard ordering of Ni2+ andNi3+ sites: the checkerboard charge ordering with qCO =(1/2, 1/2, 0) is formed below ~480 K, and is taken overby incommensurate charge order with qCO ~ (0.44, 0.44,
0) below ~180 K.
2. Experimental details
Single crystals of La1.5Sr0.5NiO4 were grown by thefloating-zone method. Four crystal rods, each of whichis ~5 mm in diameter and ~30 mm in length, were assembled for the present work. The crystal structure is
tetragonal with the space group I4/mmm. The INS measurement was performed on the chopper spectrometer
4SEASONS. The incident energy was Ei = 111 meV withenergy resolution of 10 meV at the elastic scattering
condition. We aligned the crystals so that the [001] axis
was parallel to the incident beam and the [110] axis wasin the horizontal plane.

18

3. Results and discussion
Figure 1 shows the intensity maps at 5 K as functionsof Q (momentum transfer) and ħω (energy transfer) for
several directions in the two-dimensional reciprocal lattice. Clear excitations by phonons were observed in theenergy region between ~70 meV and ~90 meV, where
the in-plane modes of phonons were observed in previous studies [1–6]. Figures 1(a) and 1(b) reflect scatteringfrom the longitudinal optical (LO) modes along [100]and [110], while Figs. 1(c) and 2(d) reflect that from thetransverse optical (TO) modes along [100] and [110],respectively. We also indicate the energies of phonons
observed in La2NiO4 along the equivalent directions(circles) [3]. The energies of the LO modes in La2NiO4
show weak Q dependences both along [100] and [110][Figs. 1(a) and 2(b)]. In contrast, the scattering spectraof La1.5Sr0.5NiO4 show quite different dispersions from
La2NiO4. There are large Q dependences with minimum
energies of ~73 meV at H = 0.5 in both directions. On
the other hand, for the TO modes in Figs. 1(c) and 1(d),the observed dispersions are almost similar to La2NiO4,
though the energies are slightly higher. The hole doping and charge ordering do not affect the energies of
the TO modes except for slight hardenings.
The observed anomalies in the LO modes as well as
their minimum energies at ~73 meV are apparently similar to those observed in x = 0.31 [6]. The similarities support the idea proposed by Tranquada et al. for x = 0.31 [6]that the doped holes cause local effects on the bondstretching phonons independent on the hole concentration. However, there is some difference between the twocompounds. In x = 0.5, the dispersion of the LO modealong [110] shows a clear softening with its minimum at(0.5, 0.5) [Fig. 1(b)], while a splitting into two modes wasobserved in x = 0.31. The difference between the present
x = 0.5 sample and x = 0.31 may be related to the difference in types of the charge ordering. In the case of thecheckerboard charge ordering in x = 0.5, the holes enter every two Ni sites, and Ni2+ sites and Ni3+ sites always
share the in-plane O ions. Therefore, the vibrations of
the shared in-plane O ions may become more coherent
along the direction of the charge-ordering wave vector,[110], resulting in the softening of the dispersion.
4. Summary
We performed an INS study on La1.5Sr0.5NiO4 to investigate the effects of hole doping on the high-energy
phonon modes. We found that the longitudinal modes

MLF Annual Report 2014

Research and Development Highlights

Figure 1. Intensity map of the high-energy excitations in La1.5Sr0.5NiO4 at 5 K on the Q-ħω planes. The intensity ismultiplied by ħω for clarity in a high ħω region. The background of the intensity was estimated from theintensity in the region of 0.9 < H < 1.1 and −0.1 < K < 0.1, and then was subtracted from the data [7].

show clearly different dispersions compared with
La2NiO4. In particular, the longitudinal mode along thedirection diagonal to the Ni square lattice shows a clear
softening, in contrast to x = 0.31 where the mode showsa splitting [6]. We interpret the difference in the phonon
anomalies between x = 0.5 and x = 0.31 as the differencein the type of charge ordering.
References[1] D. Reznik, Advances in Condensed Matter Physics
2010, 523549 (2010).
[2] D. Reznik, L. Pintschovius, M. Ito, S. Iikubo, M. Sato,
H. Goka, M. Fujita, K. Yamada, G. D. Gu, and J. M.
Tranquada, Nature 440, 1170 (2006).

[3] L. Pintschovius, W. Reichardt, M. Braden, G.
Dhalenne, and A. Revcolevschi, Phys. Rev. B 64,
094510 (2001).
[4] L. Pintschovius, J. M. Bassat, P. Odier, F. Gervais, G.
Chevrier, W. Reichardt, and F. Gompf, Phys. Rev. B
40, 2229 (1989).
[5] R. J. McQueeney, J. L. Sarrao, and R. Osborn, Phys.
Rev. B 60, 80 (1998).
[6] J. M. Tranquada, K. Nakajima, M. Braden, L.
Pintschovius, and R. J. McQueeney, Phys. Rev. Lett.
88, 075505 (2002).
[7] R. Kajimoto, M. Fujita, K. Nakajima, K. Ikeuchi, Y.
Inamura, M. Nakamura, and T. Imasato, J. Phys.:Conf. Ser. 502, 012056 (2014).

R. Kajimoto1, M. Fujita2, K. Nakajima1, K. Ikeuchi3, Y. Inamura1, M. Nakamura1, and T. Imasato4
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute for Materials Research, Tohoku University; 3Neutron
R&D Division, CROSS-Tokai; 4Department of Physics, Tohoku University

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Special Spin Density Distribution in T'-sturctured
Cuprate Oxides Studied by μSR
1. Introduction
For the emergence of superconductivity in the electron-doped cuprate oxide, both substitution of cations
such as Ce4+ at a rear-earth site and annealing procedure
under the oxygen reduction condition are required [1].
Although magnetism is recognized to play a key role inthe mechanism of superconductivity, the effects of Cedoping and oxygenreduction on the spin correlation
are not fully understood. In order to clarify these effects
on magnetism, we studied the static spin correlations in
as-sintered and annealed Pr1.40−xLa0.60CexCuO4−y (PLCCO)
by means of the muon spin rotation/relaxation (μSR)
technique. We confirmed the existence of two rotation components in both as-sintered and annealed x =0 samples, while only a single rotation component remains in the as-sintered x = 0.16 sample. These results
strongly suggest a distinct effect between annealing
and Ce-doping on magnetism. From these observations
and the numerical analysis of the internal magnetic fieldat muon stopping sites (See Fig. 1), we concluded thatat low temperatures both Cu and Pr spins form order in
the as-sintered and annealed Pr1.40La0.60CuO4−y throughthe Cu-Pr spin interaction, although the magnetic moment is reduced by annealing. In contrast, because of
the suppression of Cu-Pr interaction by electrondoping,
only the Cu spins on CuO2 planes possess the magnetic

Figure 1. Magnetic structure of Pr2CuO4 (left) and the calculated internal magnetic field (right). The gray circles
represent the possible muon stopping area evaluated from Hartree potential derived from density
functional theory (DFT) calculation. The experimentally determined magnetic field is consistent withthe calculated one for these positions.

20

transition in the highly electron-doped and as-sinteredPr1.40La0.60CuO4−y at a low temperature. These results
are consistent with the previous neutron diffraction
measurement [2], meaning that the numerical analysis
works quite well for evaluation of magnetism and will
be a powerful tool to determine the precise magnetism
such as the spin density distribution. To further confirm
the origin of the two components in the PLCCO and to
expand our study based on the numerical analysis, we
performed zero-field μSR measurement on the as-sintered Eu2CuO4 and the transversemagnetic- field μSR
measurements on PLCCO (x = 0 and 0.16).
2. Experiment
All powder samples were prepared by a conventional solid-state reaction method. We checked the phase
purity by X-ray diffraction measurement. Zero-field μSR
measurement was performed on the D1 instrument installed at the Materials and Life Science Experimental
Facility (MLF) in J-PARC. For all samples, the temperature was lowered down to 12 K and a transverse magnetic field up to 1000 Oe was applied for PLCCO.
3. Results and discussion
Figure 2 shows the muon polarization rate along
the field direction (Pz) as a function of the magnetic field(Bext) for the as-sintered x = 0 and 0.16 samples, which
was evaluated after the analysis of μSR time spectrum
at each magnetic field. The result for x = 0 cannot be
reproduced by a simple model with a single value forthe magnetic field. This suggests the existence of plural muon stopping sites with different magnetic fields.
In fact, the field dependence of Pz is well reproducedby taking the two values for the magnetic field into account. On the other hand, in the x = 0.16 sample, Bextdependence of Pz is reasonably fitted by a model witha single magnetic field at muon site(s). Figure 3 shows
the amplitude of rotation frequency obtained from a
Fourier transform of muon time spectrum, which corresponds to the density of state for the internal magnetic
field. The field distribution in Pr1.40La0.60CuO4 shows two
well-defined peaks, while that in Pr1.24La0.60Ce0.16CuO4
has a broad single peak, consistent with the analysis
of Bext-dependence of Pz. Interestingly, the field distribution in the as-sintered Eu2CuO4 shows a sharp
single peak, which is a stark contrast to the spectrum

MLF Annual Report 2014

1.0

6

2

(a)

0.6

0

Pr1.40La0.60CuO4

−2

0.2

Real amplitude

0.4

Pz

(a)

4

0.8

Pr1.40La0.60CuO4

0
0.8

(b)

8
4

Pr1.24La0.60Ce0.16CuO4

0

(b)

0.6

(c)

10

0.4

Eu2CuO4

5

0.2
0Research and Development Highlights

0Pr1.24La0.60Ce0.16CuO4
0

200

400

600

800

1000

Bext (Oe)

−5

0

1

2

3

4

5

frequency (MHz)Figure 2. Field-dependence of muon polarization rate
for the as-sintered (a) Pr1.40La0.60CuO4 and (b)Pr1.24La0.60Ce0.16CuO4 samples.

Figure 3. Real part of Fourier transform of muon time
spectrum for the sintered (a) Pr1.40La0.60CuO4, (b)Pr1.24La0.60Ce0.16CuO4 and (c) Eu2CuO4 measured at
12 K.

in Pr1.40La0.60CuO4. The different field distribution in the
two undoped compounds indicates that its origin is
attributed to the size of the rare earth moment. Then,
we calculated the internal magnetic fields at the twodominant muon stopping sites and confirmed that thecomparable magnetic fields are indeed induced at themuon sites in the T'-structured cuprate with non-magnetic rear earth ion. With increasing the size of the rearearth moment, the difference in the magnetic field at
the two muon sites increases substantially. The evaluated internal magnetic field from the magnetic structure
shown in Fig. 1(a) with the ordered moment of 0.40 μB
and 0.08 μB for Cu and Pr moments [2] can consistently
reproduce both Bext-dependence of Pz and the μSR time
spectrum in the as-sintered Pr1.40La0.60CuO4. This evaluation of the internal field at the muon sites further suggests the negligible contribution from the Pr momentin Pr1.24La0.60Ce0.16CuO4. Since the electron carrier isdoped by Ce substitution, the mobile carriers degrade
the magnetic interaction between Pr and Cu spins, possibly resulting into the paramagnetic fluctuation of thePr moment.
So far, the magnetic properties are analyzed withthe assumption that the spins are located on the atomic
positions. However, the present result suggests that the
combination between the precise μSR measurement
and the numerical analysis based on the density functional theory (DFT) calculation potentially provide a
new way to study the spin density distribution, which
represents the hybridized orbitals, in a real compound.
Although we could not carry out the measurement onannealed Eu2CuO4 and as-sintered Eu2−xCexCuO4 within
the limited beam-time, the observation of precise μSRtime spectrum in these compounds without the effectfrom the rare earth moment could give conclusive information about annealing and Ce-doping effects on
the intrinsic spin correlations on CuO2 planes.
The DFT calculation was performed under the Large
Scale Simulation Program No.14/15-13 (FY2014-2015)
of High Energy Accelerator Research Organization(KEK).
References[1] Y. Tokura et al., Nature 337 (1989) 345-347, H. Takagi
et al., Phys. Rev. Lett. 62 (1989) 1197-1200.
[2] M. Matsuda et al., Phys. Rev. B 42 (1990) 10098.

M. Fujita1, K. Tsutsumi2, K. Sato2, M. Miyazaki3, K. M. Kojima3, and R. Kadono3
Institute for Materials Research, Tohoku University; 2Depertment of Physics, Tohoku University; 3Muon Science Laboratory, High Energy
Accelerator Research Organization (KEK)121

Research and Development Highlights

MLF Annual Report 2014

Magnetic Model in Multiferroics NdFe3(BO3)4 Investigatedby Inelastic Neutron Scattering
1. Introduction
For over a decade, the coexistence of magnetic
and dielectric orders, multiferroics, has attracted significant interest in the field of condensed matter physics.
Rare-earth ferroborates RFe3(BO3)4 (R = Y, and rare-earth
metal) are a series of new multiferroic compounds containing R3+ (4f n) and Fe3+ (3d5 S = 5/2) as magnetic ions.
They exhibit a diverse magnetoelectric (ME) effect as afunction of the R3+ ions due to the variety of the magnetic anisotropy of the R3+ moments that are combined
into Fe3+ framework through the interaction between
the Fe3+ and R3+ moments (f-d coupling) [1]. Recent
studies revealed that the mechanism of magnetoelecricity in these compounds was explained by the spindependence metal-ligand hybridization model [2,3].
We focus on NdFe3(BO3)4, where the Nd3+ ions (4f 3)
carry a magnetic moment with J = 9/2. Figure 1 shows
the crystal structure with the trigonal symmetry R32.
Studies in the heat capacity, magnetic susceptibility [4]and ME effect [1] revealed that an easy-plane type antiferromagnetic (AF) order and a spontaneous electric
polarization simultaneously appear at TN = 30 K and ahuge electric polarization was induced by a magnetic
field. A neutron diffraction study exhibited the collinear
magnetic structure with propagation vector k = (0, 0,3/2) [5] as shown in Fig. 1.
In the present study, inelastic neutron scattering(INS) was performed to explore the magnetic excitations and to identify the magnetic model in NdFe3(BO3)4.
The identification of the magnetic model is essential
to understand the mechanism of multiferroicity in
NdFe3(BO3)4.

2. Experimental details
Single crystals of NdFe3(11BO3)4 were grown by a flux
method. 22 pieces of the single crystals were coaligned
so that the crystallographic a*−c* plane was horizontal. The alignment was performed by transmission Lauemethod using a high energy x-ray Laue camera. We
placed the crystals on an aluminum holder.
The INS experiment was performed at the High
Resolution Chopper Spectrometer (HRC) installed at
MLF/J-PARC. We used a closed cycle cryostat to achieve
T = 15 K. The energy of the incident neutron beam was
Ei = 11.46 meV yielding an energy resolution of ΔE =0.3 meV at the elastic position. Initially we set an incident neutron beam with ki // a* at 15 K. In order to covera wide q-range, INS spectra were collected by rotating
the crystal by 70 degrees in 2-degree steps.
3. Experimental results
Figures 2(a) and 2(b) show the INS spectra at 15 K
projected onto the ħω-(0, 0, l) and ħω-(h, 0, −1.5) planes,
respectively. We clearly observed spin waves of the Fe3+
moments around q = (0, 0, −1.5) with an energy gap of
0.57 meV, indicating the existence of an in-plane magnetic anisotropy. In addition, we observed a flat excitation at 0.98 meV, which is the transition between thelifted states of Kramers doublet of the Nd3+ ion. The spinwaves of the Fe3+ moments were more dispersive along
the c* direction than that along the a* direction, meaning that the intrachain interaction along the c-axis wasstronger than the interchain interaction. The peak energies, which were obtained by fitting using Gaussianfunctions, are plotted as open circles in Figs. 2(a) and2(b). The white circles around q = (0, 0, −1.5) exhibit ananti-crossing between the spin wave of the Fe3+ moments and the flat mode of the Nd3+ moments, implyingthat the Fe3+ moments interact with the Nd3+ moments.
4. Analysis and discussion
In order to identify the magnetic model, we consider the following Hamiltonian [6]:H = − ∑ J1 Si ⋅Sj − ∑ J2 Si ⋅Sjn.n.

n.n.n.

n.n.

k− ∑ J3 Si ⋅Sk + ∑ HCF (Jk)
Figure 1. The crystal structure and magnetic structure of
NdFe3(BO3)4 (trigonal, space-group R32) [6]. Copyright2015 by American Physical Society.

22

(1)

where the x-axis is parallel to the crystallographic a-axis
and the z-axis is parallel to the c-axis. J1 and J2 are theMLF Annual Report 2014

Research and Development Highlights

Figure 2. Color maps of the inelastic neutron scattering spectra obtained at HRC, along the (a) l and (b) h directions at 15 K. The open
circles are the peak positions extracted Gaussian fits and the curves are the calculated spin wave dispersions. Fitting curves
reasonably reproduce the experimental data [6]. Copyright 2015 by the American Physical Society.

exchange interactions in the nearest and 2nd neighborpaths of the Fe3+ ions. These terms mainly determine thedispersion along the c*-axis and a*-axis, respectively. J3 isthe nearest neighbor exchange interaction between the
Fe3+ and Nd3+ moments, which induces the anti-crossing
between the Fe3+ and Nd3+ modes. HCF is the crystal field
Hamiltonian of the Nd3+ ion, which leads to the anisotropy gap. We calculated the dispersions by a method described in Ref. [6]. The calculated dispersions are indicatedby the solid curves in Figs. 2(a) and 2(b). The fit to the data
provides excellent agreement with the overall spectrum.
In NdFe3(BO3)4, the in-plane magnetic anisotropy
plays a key role in the emergence of the multiferroicity [2].
Thus, we discussed the origin of the in-plane anisotropy
in this system as far as the crystal symmetry is preserved.
We considered possible magnetic anisotropies in theab-plane of the Fe3+ moments, the magnetic-dipole interaction, single-ion anisotropy, and the polarizationinteraction. The discussion demonstrated that none ofthese anisotropies leads to the in-plane anisotropy. The
direction of the Fe3+ moment, therefore, is determinedby the anisotropy of the Nd3+ moment through the f-d
coupling. It is interpreted from this discussion that themagnetic anisotropy of the Nd3+ moments by the crystal
field drives the multiferroicity in NdFe3(BO3)4.

5. Conclusion
INS measurements on the single crystals
NdFe3(11BO3)4 were performed to explore the magnetic excitations. The obtained spectra were successfully analyzed by spin-wave calculation. We identified
the magnetic model, where the Fe3+ moments form
strongly coupled chains along the c direction and thechains are weakly coupled in the ab–plane, the Fe3+ andNd3+ moments are strongly coupled, and the crystal
electric field of the Nd3+ ion leads the anisotropy gap.
The discussion of the origin of the in-plane magnetic
anisotropy reveals that the crystal filed of the Nd3+ ion
is a driving force in the induction of multiferroicity in
NdFe3(11BO3)4.
References[1] A. M. Kadomtseva et al., Low Temp. Phys. 36, 511(2010).
[2] A. I. Popov et al., Phys. Rev. B 87, 024413 (2013).
[3] T. Kurumaji et al., Phys. Rev. B 89, 195126 (2014).
[4] N. Tristan et al., J. Magn. Magn. Mater. 316, 621(2007).
[5] M. Janoschek et al., Phys. Rev. B 81, 094429 (2010).
[6] S. Hayashida et al., Phys. Rev. B 92, 054402 (2015).

S. Hayashida1, M. Soda1, S. Itoh2, T. Yokoo2, K. Ohgushi3, D. Kawana1, H. M. Rønnow1,4, and T. Masuda1
The Institute for Solid State Physics, The University of Tokyo; 2Neutron Science Section, Materials and Life Science Division, J-PARC center
Institute of Materials Structure Science; 3KEK, Department of Physics, Tohoku University; 4Laboratory for Quantum Magnetism, École
Polytechnique Fédéral Lausanne

123Research and Development Highlights

MLF Annual Report 2014

Crystal Field Excitations in Breathing Pyrochlore Ba3Yb2Zn5O11
1. Introduction
Geometrical frustration in magnetic materials disturbs the development of long-range order and induces
novel states at low temperatures [1, 2]. A three-dimensional network of corner- sharing tetrahedra, i.e., the pyrochlore lattice, is one of the most interesting systems.
The geometrical configuration prohibits the arrangement of the spins that satisfies the lowest energy ofall spin bonds, leading to the ground state sensitive toperturbations including single-ion anisotropy, two-ion
anisotropy, and lattice distortion. Indeed the variety ofthe magnetic phases have been reported in rare-earth
pyrochlore compounds in R2Ti2O7 [3]. In case of R = Dy
and Ho spin- ice states emerge[4] due to the geometrical frustration induced by ferromagnetic interaction
and the Ising anisotropy [5-8]. In contrast in Yb2Ti2O7 theeasy-plane type anisotropy of Yb ion enhances quantum effect, leading to quantum spin liquid state.
In a series of pyrochlore titanates R2Ti2O7 rare earth
ions carry magnetic moment. The J multiplets of theions are lifted by crystalline electric field (CEF) from octahedral ligands with the point symmetry D3d. In caseof R = Dy, Ho, and Yb, the ground state is doublet andthe first excited energies are larger than 20 meV [4],meaning that the degree of freedom of the magnetic
moments are approximately two in the temperature
range of T << 200 K. The magnetic moments are, thus,
regarded as pseudospins S = 1/2 with anisotropies determined by the wave functions of the ground state.
In most cases the localized orbitals of f-electrons givesmall magnetic interactions, and, therefore, insulating
rare-earth mag- nets are regarded as interacting spin
systems at low temperatures. Since the spin anisotropy
is one of key features for the emerged magnetic state,experimental study on CEF is crucial particularly for the
initial stage of the research on rare-earth magnets.
Breathing pyrochlore lattice, i.e., alternating arrays of corner-sharing large and small tetrahedra, isinteresting in terms of realization of the perturbative
expansion method in theoretical calculation [5]. The
original model compounds were reported in 3d-transition metal spinels LiInCr4O8 and LiGaCr4O8 [6]. Recently
rare-earth-based compound was found in Ba3Yb2Zn5O11
where Kramers ion Yb 3+ carries pseudospin S = 1/2 [7].
Fig. 1(a) shows the breathing pyrochlore network of
Yb 3+ ions. Distances between Yb 3+ ions of small andlarge tetrahedra are 3.3 A and 6.2 A, respectively. The
space group is F-43m with cubic symmetry. The local
24

structure of YbO6 is a distorted octahedron with theC3v point group symmetry as shown in Fig. 1(b). No
phase transition were observed in the specific heat andmagnetic measurement in 0.4 K < T < 300 K. A temperature dependence of the magnetic susceptibility
was reasonably reproduced using cubic symmetry for
the CEF Hamiltonian down to 30 K, even though YbO6
originally exhibited lower symmetry. This indicated that
local distortion of aYbO6 octahedron is small enoughto be approximated as a structure with cubic symmetry. It has been reported that the ground state of CEF
Hamiltonian was a Kramers doublet, and that the firstexcited state was a quartet state having an excitationenergy of 45.1 meV [7]. Up to room temperature, theexcitation energy was sufficiently high so that Yb3+ moment was regarded as an isotropic pseudospin S = 1/2.
The bulk magnetic properties in the low temperatures
were explained by the presumed isotropic Heisenberg
S = 1/2 model having non- magnetic ground state. For
the further understanding of the ground state, however, the information of the spin anisotropy is importantand, therefore, the investigation on the CEF is indispensable. In the present study, we performed inelastic
neutron (INS) scattering measurement to observe the
CEF excitations.

Figure 1. Crystal structure of Ba3Yb2Zn5O11 . (a) Breathing pyrochlore network of Yb3+ ions. (b) Local structure of
YbO6 , which has C3v symmetry. The symmetry axis
is [1 1 1].

2. Experimental details
The inelastic neutron scattering measurement(INS) was performed by using high resolution chopper
spectrometer (HRC) installed in J-PARC/MLF. We used
17.7 g powder sample synthesized by a solid state reaction method. The sample was set in an Al-can filledwith exchange He gas. Measurements were performed
at T = 3, 200 and 300 K using an 4 He-type closed-cycle
refrigerator. The T0 chopper for the elimination of fastneutrons was set at 50 Hz. The initial neutrons wereMLF Annual Report 2014

monochromated by type “S” Fermi chopper with thefrequency of 600 Hz to obtain the neutron energy of
Ei = 154.4 meV with the instrumental resolution (fullwidth at half maximum, FHWM) of 5.5 meV at the elastic position.
3. Results and discussion
Figure 2(a), (b), and (c) show contour maps of the
INS spectrum at T = 3, 200, and 300 K, respectively.
The arrows indicate three dispersionless excitations at
38.2, 55.0 and 68.3 meV. The intensities of these excitations decrease with the increase of Q, and they decrease with the increase of the temperature. None of

Research and Development Highlights

the excitation-energy values changes in the observed
temperature range. These behaviors are consistent withthat of excitations of a magnetic cluster. At ħω < 30 meV
we observed broad excitation of which the intensity increases with the Q, and it increases with the temperature. The excitation is, thus, regarded as phonons. At ħω
= 100 meV flat stripe is observed in Fig. 2(a). Since nointensity was observed at 100 meV in preliminary measurement at MARI (not shown), the stripe is regarded as
artifact. The intensities decrease with the increase of Q,
and they follow the magnetic form factor of the Yb 3+
ion indicated by the solid curves [8]. These excitations,thus, derive from the CEF of the Yb3+ ion. Contour mapsof INS spectra measured at at (a) T = 3, (b) T = 200, and(c) T = 300 K. The arrows indicate dispersionless excitations at ħω = 38.2, 55.0 and 68.3 meV. ground state decreases with the increase of the temperature and theoccupancy is one of coefficients in magnetic neutron
cross section, all of the excitations derive from the transitions between the ground state and excited states.
This means that the Yb3+ ion is the four-level system as
described by solid bars in the first row in Fig. 3. The result is in contrast with the three level system assumed
in the previous study [7] as described by dotted bars inthe second row. The first excited energy of the present
study is, however, close to that of previous one.
4. CONCLUSION
We performed a neutron scattering experiment on
a powder sample of Ba3Yb2Zn5O11 in order to identify
the CEF Hamiltonian. The neutron spectrum was explained by four Kramers doublets of Yb3+ ion.

Figure 2. Contour maps of INS spectra measured at at (a) T =3, (b) T = 200, and (c) T = 300 K. The arrows indicate
dispersionless excitations at ħω = 38.2, 55.0 and
68.3 meV.

Figure 3. Energy diagrams of Yb3+ compounds, Ba3Yb2Zn5O1112), Yb2Ti2O7 4) and YbBa2Cu3O7 15). The solid anddotted lines indicate the levels obtained by neutron scattering studies and bulk measurement, respectively.

25

Research and Development Highlights

MLF Annual Report 2014

References[1] A. P. Ramirez, Annu. Rev. Mater. Sci. 24, 453 (1994).
[2] L. Balents, Nature 464, 199 (2010).
[3] J. S. Gardner, M. J. P. Gingras, and J. E. Greedan, Rev.
Mod. Phys. 82, 53 (2010).
[4] A. Bertin, Y. Chapuis, P. D. Reothier, and A. Yaouane,
J. Phys.: Condens. Matter 24, 256003 (2012).
[5] H. Tsunetsugu, Phys. Rev. B 65, 024415 (2001).
[6] Y. Okamoto, G. J. Nilsen, J. P. Attfield, and Z. Hiroi,

Phys. Rev. Lett. 110, 097203 (2012).
[7] K. Kimura, S. Nakatsuji, and T. Kimura, Phys. Rev. B
90, 060414 (2014).
[8] P. J. Brown, International tables for crystallography(John Wiley and Sons, Inc, 2006) 1st online ed., Vol.
C, p. 454.
[9] M. Guillaume, P. Allenspach, J. Mesot, et al., Solid
State Commun.81, 999 (1992).

T. Haku1, M. Soda1, M. Sera2, K. Kimura2, S. Itoh3, T. Yokoo3, and T. Masuda1
Institute for Solid State Physics, The University of Tokyo, Kashiwa, Chiba 277-8581, Japan; 2Division of Materials Physics, Graduate
School of Engineering Science, Osaka University, Toyonaka, Osaka, 560-8531, Japan; 3Institute of Materials Structure Science, High Energy
Accelerator Research Organization, Tsukuba, Ibaraki, 305-0801, Japan1

26

MLF Annual Report 2014

Research and Development Highlights

Magnetic Excitations in the γ-FeMn Itinerant Electron
Antiferromagnet
1. Introduction
There is a theoretical assumption that the magnetic
excitations in itinerant electron magnets consist mainlyof spin-wave excitation and Stoner excitation. The former
is a collective excitation and the latter is a single-particle
excitation. The spin-wave excitation localizes in the momentum Q space, and has dispersion relation between
Q and the excitation energy ħω. On the other hand, theexcitation spectrum of the Stoner excitation forms continuum. The dispersion curve of the spin-wave excitation enters into the continuum of Stoner excitation at a Q point,
and is strongly damped by the coupling with the Stonerexcitation. Inelastic neutron scattering is a powerful toolfor exploring magnetic excitations, because it can observe
the imaginary part of the dynamical magnetic susceptibility Imχ in Q and the ħω space. In one of the itinerant
electron ferromagnets, MnSi, the magnetic excitations,as described above, were observed experimentally byneutron scattering [1]. On the other hand, in itinerant
electron antiferromagnets, a full picture of the magnetic excitations has yet to be revealed. One of the typicalitinerant electron antiferromagnets is Cr metal. A recent
calculation based on a multiband Hubbard model has
predicted that the spin-wave excitation damps up to ~0.6 eV [2]. Experimentally, the magnetic excitations in Cr
have been revealed only up to ħω = 0.25 eV [3], because
it is difficult to measure excitations of sub-eV energy region. By the low-energy (ħω < 0.1 eV) excitation studies,it has been established to date that the spin-wave dispersion in itinerant electron antiferromagnets has steep
and isotropic character. However, the spin-wave dispersion near the magnetic zone boundary is unknown,
and it can be anisotropic like that in the Heisenberg
spin system. In addition, it remains unclear whether thestrong damping of the spin-wave excitation occurs. This
limitation is due to the steep character of the spin-wave
excitation. Therefore, we focused another typical itinerant electron antiferromagnet, γ-FeMn. The steepness ofthe spin-wave dispersion was determined to be moderate(160-250 meVÅ) [4] compared to that of Cr. Additionally, it
was reported that the scattering intensity became weakat ħω = 54 meV [5], suggesting that the spin-wave damping may be observed at excitation energy lower than thatof Cr. γ-FeMn has a face-centered cubic structure. The Fe
ions, which are located at the face-centered position, havemagnetic moments, and form non-coplanar magnetic

structure under the transition temperature between 400
and 500 K [6]. In this study, we performed inelastic neutron scattering measurement in γ-FeMn.
2. Experiments
A single crystal of Fe0.7Mn0.3 was aligned in the hkk
zone. The volume of the sample was about 5 cc. The
sample was sealed in an aluminum can in He gas atmosphere. Inelastic neutron scattering experiments were
performed at the High Resolution Chopper Spectrometer
installed at BL12 beamline, J-PARC/MLF. The incident neutron energy Ei was selected as 33, 82 and 206 meV. The energy resolution at the elastic scattering position was 1.2,
4 and 15 meV, respectively. A closed cycle 4He refrigerator was used to cool down the sample to temperature T= 14 K.
3. Results and discussion
The ħω dependence of Imχ at a magnetic zone center Q = (0, −1, −1) measured with Ei = 33 meV is shownin Fig. 1. The energy gap of Eg = 10.2(7) meV was confirmed, a result which was consistent with the previous
report [4]. The ħω dependence of Imχ monotonically increased, which was different from the Heisenberg spin
system. The scattering intensity map along [0, −k, k] and[h, 0, 0] around at Q = (0, −1, −1) and ħω = 75 meV with
Ei = 206 meV is shown in Fig. 2, indicating the isotropic
nature of the magnetic excitation. The data analysis along[001], [011] and [111] directions revealed that the excitation was isotropic in all three directions. The measurement
performed around at ħω = 48 meV with Ei = 82 meV indicated a similar result (not shown). Strong damping or

Figure 1. ħω dependence of Imχ at Q = (0, −1, −1).

27Research and Development Highlights

MLF Annual Report 2014

Figure 2. The scattering intensity map around at Q = (0, −1, −1)and ħω = 75 meV.

Figure 3. The spin-wave dispersion of γ-FeMn.

broadening of the dispersion curve was not found up
to ħω = 75 meV. The spin-wave dispersion is summarized in Fig. 3. The dispersion was found to be steeper
than the one previously reported [4], and similar to thatof Fe0.47Mn0.53 [5]. The dispersion at ħω = 75 meV was Q =0.24 Å−1, which is still far from the zone boundary of about
0.9 Å−1.

excitations, measurements at a higher excitation energy are required.

4. Summary
Magnetic excitations in γ-FeMn itinerant electron
antiferromagnet were investigated by the neutron
scattering technique. The spin-wave dispersion was
isotropic and did not show strong damping up toħω = 75 meV. To reveal a full picture of the magnetic

References[1] Y. Ishikawa, J. Appl. Phys. 49 (1978) 2125.
[2] K. Sugimoto, Z. Li, E. Kaneshita, K. Tsutsui and T.
Tohyama, Phys. Rev. B 87 (2013) 134418.
[3] S. Itoh, H. Hiraka et al, KENS REPORT 19 (2012) 17.
[4] K. Tajima, Y. Ishikawa, Y. Endoh and Y. Noda, J. Phys.
Soc. Jpn., 41 (1976) 1195.
[5] Y. Endoh, G. Shirane, Y. Ishikawa and K. Tajima, Solid
State Comm. 13 (1973) 1179.
[6] Y. Endoh and Y. Ishikawa, J. Phys. Soc. Jpn. 30 (1971)
1614.

S. Ibuka1,2, T. Yokoo1,2, S. Itoh1,2, and Y. Endoh2,3
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3Tohoku
University
1

28

MLF Annual Report 2014

Research and Development Highlights

Anomalous Magnetic Response in the Overdoped
Checkerboard Ordered Phase of Layered Nickel Oxides
Nd2-xSrxNiO4
1. Introduction
The stripe-type charge spin ordering, which emerges in the layered transition-metal oxides resulting fromcarrier doping, has attracted wide attention because of
its close relationship with the high-Tc superconductivity in La2−xSrxCuO4 [1]. In particular, it is of great importance to understand the spin dynamics of the layeredtransition-metal oxides through wide hole concentrations from an antiferromagnetic Mott-insulating region
to a fully metallic overdoped region. In this regard, thelayered nickel oxide RE2−xSrxNiO4 (RE: rare earth) is oneof the most noteworthy systems, where the diagonal
stripe ordering appears in a wide insulating hole concentration range (~1/3 ≤ x ≤ ~1/2), as observed in previous
systematic neutron scattering studies [2, 3]. For nickel
oxides, the stripe ordering is characterized by diagonallysegregated hole stripes (Ni3+: S = 1/2) separating the antiferromagnetic spin order (Ni2+: S = 1) as a domain boundary (see Fig. 1(a)). Above x ~ 0.5, the doped holes are still
highly correlated, and then they are alternately localized on the nickel sites at low temperatures and form astatic checkerboard (CB)-type charge (spin) pattern, as
shown in Fig. 1(b). Such CB-type charge spin ordering in
Nd2−xSrxNiO4 persists up to the insulator-to-metal transition x ~ 1.0 [2, 3], although the electronic conductancegradually increases with hole doping [3, 4].
As already known, the magnetic excitation spectra in
the Mott-insulating antiferromagnetic region (La2NiO4; x= 0) can be explained by the 2D linear spin wave (LSW)
theory [5]. Similarly, the qualitative features of the spin
dynamics in the stripe ordered region (x ~ 1/3) can also
be well reproduced by the 2D LSW theory [6]. Meanwhile,
Freeman et al. observed broad magnetic excitation spectra for the CB ordered x = 1/2 sample (La3/2Sr1/2NiO4).
Although they argued that the observed excitations
can be approximately explained within the frame workof the LSW theory [7], the existence of any differencesin the spin dynamics between the stripe and the overdoped CB ordered regions still remains questionable.
When examining further the spin dynamics in the overdoped CB region, it becomes clear that a major bottleneck obstructs the growth of large single crystal samplesof the La2−xSrxNiO4 system. As an alternative strategy,
we focused on the Nd-based Nd2−xSrxNiO4 system andFigure 1. A schematic illustration of (a) stripe and (b) checkerboard type charge-spin ordering in the NiO2
planes where the doped holes (open circles) enter
into the Ni3+ sites. The arrows indicate the spins of
S = 1 on the Ni2+ sites. The parallelogram in (a) andrectangle in (b) correspond to the superstructuresof the stripe and CB ordering, respectively. (c) A diagram of the 2D reciprocal space showing the Bragg
points for the stripe and CB spin ordering characterized by the incommensurability ε. The circles andsquared symbols represent two equivalent sets of
the Bragg points from orthogonal domains in the(H, K) plane. The cross symbols indicate the antiferromagnetic zone center.

carried out inelastic neutron scattering experiments onthat system through a wide hole concentration range.
The advantage of the Nd-based system is the possibilityof growing a single-crystal for the overdoped region (x> 0.5). Furthermore, it is also convenient that magnetic
properties derived from Ni spins are fully identical between the Nd- and La-based systems, as confirmed in ourprevious studies of the Nd-based system [2, 3, 8]. In thiscolumn, we report our recent observation of the anomalous spin response in the overdoped CB ordered phase.
2. Experimental Procedure
Single crystalline samples of Nd2−xSrxNiO4 (x = 0.33,
0.60, and 0.70) were grown by a floating zone method
in a four-elliptical mirror furnace [8]. The mass of eachsingle crystal samples of x = 0.33, 0.60 and 0.70 is 18.5,
53.1 and 17.2 g, respectively. These single crystal rods
were coaligned within 0.5° by utilizing the high-energy
transmission Laue instrument installed at ISSP. Inelastic
neutron scattering experiments were performed with the29

MLF Annual Report 2014

3

4

2.0

(c) 60 < ħω < 70

[0, K] / r. l. u.

Intensity / arb. unit

0.5
0.0
-0.5

0.5 1.0 1.5[H, 0] / r. l. u.

2.0

0.5 1.0 1.5[H, 0] / r. l. u.

(f) 30 < ħω < 40

2.0

4.5

(e) 20 < ħω < 3008(d) 10 < ħω < 20

0

1

0

2.5

-1.0

7.5

[0, K] / r. l. u.

1.0
0.5
0.0
-0.5
0.5 1.0 1.5[H, 0] / r. l. u.

2.0

0

0.5 1.0 1.5[H, 0] / r. l. u.

2.0

2.5

0

4

-1.0

4.5

30

0.5 1.0 1.5[H, 0] / r. l. u.

(b) 50 < ħω < 60

1.0

4.5

3. Results and Discussion
Figures 2(a)-2(c) exhibit the constant energy slicesof the stripe ordered x = 0.33 sample at various energy
transfers. At lower energy transfers, reflected in panel2(a), clear magnetic excitations were observed at aroundthe magnetic Bragg points characterized by incommensurability ε ~ 0.36. As the energy transfer increases, thecircle-like spectrum in Fig. 2(a) changes to a ring-shaped
excitation spectrum, as seen in Figs. 2(b) and 2(c). The
peak position of the observed excitations for the x = 0.33
sample was examined by fitting the data to the Gaussianfunction and the results are plotted in Fig. 3(a). Here, one
can recognize that the magnetic excitation splits into
two counterpropagating peaks above ~40 meV, indicating the existence of the clear “V-shaped” dispersion relation for the x = 0.33 sample. The energy of the magnetic
zone boundary for the x = 0.33 sample is estimated to beabout 80-100 meV. In Fig. 3(a), the calculated spin wave
dispersion relation is also displayed by the solid anddashed lines using the same exchange parameters (J0 =2J1 = 14 meV: see also Fig. 1(a)) as those of the La-based
x = 1/3 sample [6]. As seen in Fig. 3(a), these features ofthe excitation spectra in the Nd-based x = 0.33 sample
are qualitatively identical to those of the La-based samples [6]. These results clearly indicate that the influenceof the Nd ion on the spin wave excitations of the Ni spins
is practically negligible. Consequently, these findings ensure that the study of the Nd2−xSrxNiO4 system yields results that are qualitatively identical with those obtained
from the study of the La-based system.
Next we focused on the magnetic excitation spectra
for the overdoped x = 0.60 sample in the CB ordered region. Figures 2(d)-2(f) show the constant energy slices of
the Nd-based x = 0.60 sample at various energy transfers.

(a) 40 < ħω < 50

7.5High Resolution Chopper spectrometer installed at BL12in MLF of J-PARC in Tokai. The T0 chopper was used to reduce the background noise, which originates from highenergy neutrons emitted during neutron production. An
incident collimation with 1.5° and an iron squared collimator with an aperture of 50*50 mm were used to improveincident beam collimation. The samples were enclosed in
the standard Al cell with 4He gas and cooled below 10 K
(2.5 K for x = 0.33) by utilizing the closed-cycle 4He refrigerator (PASCAL, Sumitomo). Following previous works,
we denoted the reciprocal space by the orthorhombic
notation (F4/mmm). In all measurements, the [001] direction was set parallel to the incident neutron beam (ki // c),and the measured neutron intensity was projected in the(h, k) plane as a function of the energy transfer.

00.5 1.0 1.5[H, 0] / r. l. u.

2.0

Figure 2. Constant energy contour plots of (a-c) the x = 0.33
sample (Ei ~ 165 meV, resolution ~ 15 meV, T ~2.5 K) in the stripe ordered region, and (d-f ) the x =0.60 sample (Ei ~ 124 meV, resolution ~ 10 meV, T <10 K) in the CB ordered region.

120

120

(a) H = [0.6~0.7]

ħω / meV

Research and Development Highlights(b) H = [0.5~0.6]

100

100

80

80

60

60

40

40

20

x = 0.60
T ~ 14 K

Ei ~ 71 meV
ΔE ~ 4 meV20
x = 0.33
T ~ 2.5 K

0
-1.0

-0.5

Ei ~ 165 meV
ΔE ~ 15 meV0.0

K / r. l. u.

0.5

1.0

0
-1.0

-0.5

0.0

0.5

1.0

K / r. l. u.

Figure 3. Dispersion relation of the observed magnetic excitation spectra for (a) the x = 0.33 sample (Ei ~165 meV, resolution ~ 15 meV) and for (b) the x =0.60 sample (Ei ~ 71 meV, resolution ~ 4 meV). The
solid and dashed lines in the panel (a) shows a calculation of the spin wave dispersion for the stripetype spin order model with J0 = 2J1 = 14 meV. The
solid line in the panel (b) is also a calculation for
the CB-type spin order model with J1 = J0/2. The
definition of the exchange constants is described inFig. 1(a) for the stripe order and 1(b) for the CB order.

As seen in Fig. 2(d), clear spots were observed at around(H, K) = (0.44, 0) and its equivalent positions in the Q space,suggesting that the CB-type charge-spin ordering in thex = 0.60 sample. When the energy transfer increased, theobserved magnetic excitations became broader in the
Q space in the energy range of Fig. 2(e), and began tooverlap at higher energy transfers, as shown in Fig. 2(f).
Above 60 meV, no significant magnetic excitations wereobserved in the x = 0.60 sample. Note that qualitatively
similar magnetic excitations were observed for the further overdoped x = 0.70 sample. The peak position of theMLF Annual Report 2014

observed excitations for the x = 0.60 sample is shown in
Fig. 3(b). In marked contrast to the well-defined dispersing excitation spectra observed in the x = 0.33 sample, themagnetic excitations of the x = 0.60 sample are broader
than those of the x = 0.33 sample, and they remain centered at the magnetic Bragg point up to the energy ofthe magnetic zone boundary (O ~ 40-60 meV). Namely,
no significant split of the magnetic excitation spectra wasobserved for the CB-ordered samples within the experimental resolution. We could summarize several marked
features in the observed magnetic excitations in the
CB-ordered region as follows: (i) the energy scale of themagnetic zone boundary (O ~ 40-60 meV) is roughly halfof that of the stripe ordered region, (ii) there is no significant split (dispersion relation) of the magnetic excitationin the CB region, (iii) features (i) and (ii) are qualitatively
unchanged in the CB region, at least up to x = 0.70.
As for feature (i), we consider that such a reductionof the energy scale can be attributed to the lack of J0 in
the CB region, as shown in Fig. 1(b). For feature (ii), theorigin still remains to be determined. To clarify the unusual feature of (ii) in the magnetic excitation spectra in
the CB region, further experimental and theoretical studies would be indispensable. In order to reveal the originof feature (iii), we should refer to a pioneering investigation of the orbital state of the Ni ions [4]: here, Uchida
et al. suggested that the doped holes first enter intod(x2−y2) orbital for x < 0.5 and subsequently into d(3z2−r2) for x > 0.5. Furthermore, they indicated that the site
occupancy of d(x2−y2) is kept at 50% for the CB region
up to x ~ 1.0. In Fig. 4, we visualized a possible structuralmodel of the arrangement pattern of the orbitals for the
stripe and overdoped CB-ordered regions [10] on the basis of Uchida’s results [4] and previous neutron scatteringexperiments [2, 3, 9]. This structural model can explain
the robustness of the CB-type pattern and the independence of several features in the observed magnetic excitations from the hole concentration above x > 0.5. We
believe that the orbital degrees of freedom of the Ni ionsand their arrangement pattern would be crucial to understanding the observed unusual magnetic excitationsin the overdoped CB regions in the layered nickel oxides.
4. Concluding Remarks
We investigated the magnetic excitations of the

Ni

(a)

2+

Research and Development Highlights

(b)

(c)

(S = 1)2

2

d(x -y )22d(3z -r )
Ni

3+

2

Stripe ( ε = 1/3)

2

2

d(x -y )2(d)2

Diagonal striped(x -y )-lattice
2 2+ Perfectd(3z -r )-lattice(S = 1/2)

(e)

(f)

2

d(3z -r )Ni

3+(S = 1/2)
2

2

d(x -y )22d(3z -r )Checkerboard(ε ~ 1/2, x > 0.5)22

Perfect CB d(x -y )-lattice
2 2+ Disordered d(3z -r )-lattice

Figure 4. (Cited from ref. [10]) A simplified structural model of(a-c) the x = 1/3 stripe and (d-f ) the overdoped CB
order in the layered nickel oxides. Orbital and spin
degrees of freedom of the Ni ions are illustrated in
the left side of the figure, here, d(x2-y2) and d(3z2r2) orbitals are individually drown in (b, e) and (c, f ),respectively.

stripe ordered and the overdoped CB-ordered layered
nickel oxide Nd2−xSrxNiO4. The magnetic excitations of the
stripe ordered x = 0.33 sample can be described by the
LSW theory and they are qualitatively identical to thoseof La5/3Sr1/3NiO4. In marked contrast to the clear spin wave
excitations in the stripe ordered sample, the CB-orderedsample shows unusually non-dispersive broad magnetic excitation spectra. No significant hole concentration
dependence in the features of the magnetic excitation
spectra was observed in the CB-ordered region. We investigated the origin of the robustness of the CB order abovex > 0.5 by taking into account the orbital degrees of freedom of the Ni ions. These experimental results appearedin the Journal of the Physical Society of Japan [10].
References[1] J. M. Tranquada et al., Nature 375, 561 (1995).
[2] H. Yoshizawa et al., Phys. Rev. B 61, R854 (2000).
[3] K. Ishizaka et al., Phys. Rev. B 67, 184418 (2003).
[4] M. Uchida et al., Phys. Rev. B 86, 165126 (2012).
[5] S. Itoh et al., J. Phys. Soc. Jpn. 63, 4542 (1994), andreferences therein.
[6] A. T. Boothroyd et al., Phys. Rev. B 67, 100407(R)(2003); H. Woo et al., Phys. Rev. B 72, 064437 (2005).
[7] P. G. Freeman et al., Phys. Rev. B 71, 174412 (2005).
[8] Y. Ikeda et al., J. Phys. Soc. Jpn. 84, 023706 (2015).
[9] R. Kobayashi et al., J. Phys. Soc. Jpn. 84, 064711 (2015).
[10] Y. Ikeda et al., J. Phys. Soc. Jpn. 85, 023701 (2016).

Y. Ikeda1, S. Suzuki1, T. Nakabayashi1, H. Yoshizawa1, T. Yokoo2, and S. Itoh2
Neutron Science Laboratory, Institute for Solid State Physics, The University of Tokyo; 2Neutron Science Division, Institute of Materials
Structure Science, High Energy Accelerator Research Organization, KEK

1

31

Research and Development Highlights

MLF Annual Report 2014

Nd-Substitution Effect on Metal–Nonmetal Transition in
PrRu4P12
Nd-substituted material with x = 0.20 is higher than
52.6 and 36.0 K of Pr0.8La0.2Ru4P12 and Pr0.8Ce0.2Ru4P12,
respectively [6, 7].

4500Counts / 500 sec.

1. Introduction
The metal–nonmetal transition at TM-I = 63 K of
PrRu4P12 has been studied extensively [1]. The nonmetallic phase below TM-I is characterized by the wave
vector q0 = (1, 0, 0), which indicates the structural transition from body-centered cubic to simple cubic [2].
Inelastic neutron scattering (INS) studies have proventhat the nonmetallic phase is associated also with theq0 alignment of two inequivalent crystal-field (CF) level
schemes of the Pr-ion 4f 2 state: a singlet at Pr1 and a
triplet at Pr2 at the lowest temperature [3]. This phasetransition was interpreted as charge-density-wave(CDW) formation, which is accompanied by the antiferro-type ordering of an f-electron totally symmetricmultipole [4, 5]. It is worth noting that a reentrant-typephase transition is induced by substituting Ce to Pr [6].
The ordered state appears once at TM-I ~ 45 K, and disappears below approximately 10 K. The atomic substitution, which corresponds to carrier doping, destabilizes
the multipole-ordered nonmetallic phase [7]. On theother hand, the triplet state at Pr2 in the nonmetallic ordered phase is considered controversial because of its
finite entropy owing to the degeneracy. This fact raises
the question of magnetic perturbation’s influence on
the ordered state.
In order to investigate the magnetic-impurity effect on the order of PrRu4P12, we studied the CF schemeand the superlattice of Pr1-xNdxRu4P12. The result is to be
published elsewhere [8].

Pr0.85Nd0.15Ru4P12
X-ray diffraction
Q = (9, 6, 0)

4000

TMI = 58.0 K

3500
3000
background

2500
2000

0

20

40
60
Temperature [K]

80

100

Figure 1. Temperature dependence of X-ray superlattice
peak intensity of Pr0.85Nd0.15Ru4P12 [8].

BL12 (HRC), Ei = 30.6 meV, Q = 1.5 - 2.5 Å-1
0.60(a) PrRu4P12
7.3 K
45 K
56 K

0.40

2. Experimental Procedure
Samples of Pr1-xRxRu4P12 (R = La, Ce, and Nd) weresynthesized by the Sn-flux method. We measured the
CF level schemes by using the high-resolution chopper
neutron spectrometer HRC at BL12, MLF. X-ray diffraction was performed on a four-circle diffractometer at
Tohoku University.
3. Results
We measured temperature dependences of the
X-ray superlattice reflection intensities of Pr1-xNdxRu4P12
with x = 0.05, 0.15, and 0.20. Figure 1 shows the datafor x = 0.15, in which the superlattice peak at (9, 6,0) emerges at low temperature. The TM-I of x = 0.05,
0.15, and 0.20 are determined to be 61.5, 58.0, and57.1 K, respectively. It is worth noting that TM-I of the
32

Counts (arb. units)

0.20
0.00
0.40

(b)
Pr0.85Nd0.15Ru4P12
8.5 K
44 K
56 K
Pr0.85Ce0.15Ru4P12
10 K

0.20

0.00

0

5
10
Energy [meV]15

Figure 2. Temperature dependences of INS spectra of (a) the
pure system PrRu4P12 and (b) Pr1-xRxRu4P12 (R = Ceand Nd) [8].

MLF Annual Report 2014

Figure 2 shows the INS spectra of (a) PrRu4P12 at 7.3,
45, 56 K, (b) Pr0.85Nd0.15Ru4P12 at 8.4, 44, 56 K, together
with Pr0.85Ce0.15Ru4P12 at 10 K. The spectra in the wholetemperature range below TM-I are almost identical between PrRu4P12 and Pr0.85Nd0.15Ru4P12. Therefore, themultipole order parameter at the Pr-ion sites is robust
against the Nd-ion substitution. On the other hand,
the lower-temperature spectrum of Pr0.85Ce0.15Ru4P12 ismuch broader than the pure and Nd-substituted compounds. This experimental result indicates that carriers
do not vanish because of the imperfect Fermi-surface
nesting caused by the carrier doping effect.
4. Discussion
NdRu4P12 undergoes a ferromagnetic transition at
1.6 K with an ordered magnetic moment of 1.8 μB/Nd [8].
This supports the hypothesis that magnetic moments
are introduced into PrRu4P12 by the Nd substitution.
The present INS result indicates that the ordered state
is not destroyed by the introduced Nd-ion magnetic
moments. On the contrary, the Nd substitution seems
to assist the multipole ordering because the reduction
in TM-I is less than that of the La-substituted system: TM-I
= 52.6 K for La 20%. It is indicative that a site-dilution
effect on the ordered state is overcome by the Nd substitution. A magnetic interaction between Nd and Pr is
expected to stabilize the Pr2 triplet ground state, whichshould be located at the neighbors of the introduced
Nd ion. Because the CF ground state of the Nd ions in
NdRu4P12 is a quartet, multipole degrees of freedom of

Research and Development Highlights

Nd ion may also contribute to the stabilization of thePr2 triplet. Therefore, we conclude that the multipoleordered CDW state is compatible with the magnetic
impurity.
The findings raise another question concerning
the f-electron state: how the robust multipole orderedphase in the lower Nd-concentration region crosses
over or transforms into the ferromagnetic ordered stateof the pure NdRu4P12. We are continuing the investigation of the series of Pr1-xNdxRu4P12 in a wide range of x.
References[1] C. Sekine, T. Uchiumi, I. Shirotani, and T. Yagi, Phys.
Rev. Lett. 79, 3218 (1997).
[2] C. H. Lee, H. Matsuhata, H. Yamaguchi, C. Sekine, K.
Kihou, T. Suzuki, T. Noro, and I. Shirotani, Phys. Rev.
B 70, 153105 (2004).
[3] K. Iwasa, L. Hao, K. Kuwahara, M. Kohgi, S. R. Saha,
H. Sugawara, Y. Aoki, H. Sato, T. Tayama, and T.
Sakakibara, Phys. Rev. B 72, 024414 (2005).
[4] Y. Kuramoto, J. Otsuki, A. Kiss, and H. Kusunose,
Proc. Theo. Phys. Suppl. 160, 134 (2005).
[5] T. Takimoto, J. Phys. Soc. Jpn. 75, 034714 (2006).
[6] C. Sekine, M. Takusari, and T. Yagi, J. Phys. Soc. Jpn.
80, SA024 (2011).
[7] K. Saito, C. Laulhé, T. Sato, L. Hao, J.-M. Mignot, andK. Iwasa, Phys Rev B 89, 075131 (2014).
[8] K. Iwasa, A. Yonemoto, S. Takagi, S. Itoh, T. Yokoo,
S. Ibuka, C. Sekine, and H. Sugawara, accepted by
Physics Procedia.

K. Iwasa1, A. Yonemoto1, S. Takagi1, S. Itoh2, T. Yokoo2, S. Ibuka2, C. Sekine3, and H. Sugawara4
Department of Physics, Tohoku University; 2Condensed Matter Research Center and Neutron Science Division, Institute of Materials
Structure Science, KEK; 3Department of Electrical and Electronic Engineering, Muroran Institute of Technology; 4Department of Physics,
Kobe University

133

Research and Development Highlights

MLF Annual Report 2014

Spin and Hole Dynamics in Carrier Doped Quantum
Haldane Chain
1. Introduction
In a low-dimensional system, the quantum nature of spins appears in macroscopic phenomena. A
Haldane gap is one of those unconventional propertiesof the one-dimensional (1D) integer spin systems inwhich a spin gap exists between the ground state andthe first excited state [1, 2]. Inorganic nickelate Y2BaNiO5
was found to be a good candidate for a Haldane systemwith a spin gap of 10 meV at the magnetic zone center(MZC) [3, 4]. In R2BaNiO5 (R = Nd, Pr), the observed excitation energy is quite similar to the Haldane gap in
Y2BaNiO5 and shows a structure factor reflecting a 1D
Ni chain correlation even though it displays 3D antiferromagnetic order at low temperature [5-9]. Thus, it
was found that Nd2BaNiO5 was not a simple Haldane
system.
Another topic of interest regarding the transition
metal chain oxides is carrier doping, which yields phenomena ranging from strongly renormalized Fermi liquid behavior to high-temperature superconductivity.
In view of the enhanced quantum fluctuations in 1D
systems, doping of transition metal chains could welllead to equally surprising discoveries. R2BaNiO5 is acharge-transfer insulator [10, 11], and some quantity ofhole carriers has been successfully introduced primarily into oxygen sites by replacing part of the off-chain
R3+ with Ca2+ [4]. The spin dynamics of the hole-doped
Ni 1D chains have also been addressed using a theoretical approach [12, 13] and through neutron experiments [14, 15].
In this article, we present the spin and hole dynamics of hole-doped Nd2BaNiO5 measured by means of apulsed neutron scattering technique to survey the entire area of the Brillouin zone in momentum and energy
space.
2. Experimental
The carrier content can be controlled by replacing
a portion of the Nd3+ ions with Ca2+. Lightly doped (x =0.1) Nd2-xCaxBaNiO5 was chosen for the neutron experiments. TN was evaluated as 30 K. Two cylindrical single
crystals with a total mass of 13 g were assembled in analuminum can. Three pieces of specimens with dimensions of 5 mm in diameter, and 31 to 35 mm in length
were co-aligned. A closed-cycle refrigerator was used
to cool the sample down to low enough temperature.
34

Inelastic neutron scattering experiments were conducted at the High-Resolution Chopper spectrometer (HRC)
installed at the Materials and Life Science Experimental
Facility in J-PARC [16, 17]. The measurement temperatures were 4, 20, 30, 40, and 150 K, which are above andbelow TN. Incident neutron energy Ei of 102.0 meV waschosen to measure a wide Q-E space.
3. Results
In the neutron scattering experiment, the [H 0 L]
zone was into the horizontal scattering plane, where H
corresponds to the chain direction (crystallographic aaxis). Figure 1 shows the obtained dynamical structures
S(Q,E) at T = 4.0 K (well below TN = 30 K) and T = 40 K
(above TN). Both spectra are normalized by the measurement time. Intense crystal electric field (CEF) excitationsof Nd3+ ions lie at E = 24 and 38 meV. The site symmetry of Nd3+ in Nd2BaNiO5 is sufficiently low to split thetenfold degenerate J = 9/2 multiplet into five Kramers
doublets. In addition to the CEF excitations, excellent
dispersion relations for the Ni 1D chain are observed
at both temperatures for the entire first and second
Brillouin zones. The minima of the dispersion observedat the MZC, H = 0.5, 1.5, and even 2.5, occur where themagnetic scattering intensity becomes weak becauseof the magnetic form factor, and the phonon scattering
is dominant in this high-Q region. On the other hand,at H = 1.0 and 2.0, the weight of the magnon dispersion is known to be zero at the zone boundary. At low
temperature [Fig. 1(a)], the magnon bandwidth reaches
60 meV, with somewhat large gap energy of Δ = 20 meV,compared to the bare (unperturbed) 1D Haldane gap.
In addition, a flat band lying at E = 65 meV and corresponding to a phonon or magnon optical branch wasobserved.
At T = 40 K, the Haldane gap is lowered, and thespectral weight is slightly shifted with respect to the
MZC. The boundary energy is almost the same at bothtemperatures.
To survey the spectra near the gap, constant-Q
cuts are shown in Fig. 2 for both temperatures. Because
the transfer energy in Figs. 1 and 2 is strongly related
to the wave vector parallel to the incoming neutron
beam ki (crystallographic c-axis in our experiment),
the 1D spectra are also a function of L. However, inthe 1D system, only the chain direction can be varied,MLF Annual Report 2014

Research and Development Highlights

Figure 1. Observed dispersion relation of x = 0.1 at (a) T = 4.0 K (< TN) and (b) T = 40 K (> TN). Flat bands at E = 24 and 38 meV are
contributions from crystal field excitation of Nd3+ ions. Oscillating signals showing minima at magnetic zone center (H =0.5 and 1.5) are from 1D chain. (from Ref. [18])show the detailed structure below the Haldane gap,
considerable weight was observed, indicating a holedynamical structure as an in-gap state. By analogy
with the slightly doped (x = 0.035) compound [19], theweight at the MZC (H = 0.5) appeared as a result of hole
doping. We now plan to perform further experiments
at a high-energy resolution to observe the dynamical
structure below the gap.
Thus, the entire dynamical set of properties of ahole-doped 1D Ni chain was successfully measured bypulsed neutron inelastic scattering. At TN, the dynamical structure changes dramatically, presenting new features - a local excitation at E = 10 meV and doped holedynamics below the gap energy - in addition to a viewof the entire 1D chain dispersion.

Figure 2. Energy spectra at Q = (0.5, 0, L). Open symbol is themeasurement at T = 4 K, which is well below TN.
Solid symbol is at T = 40 K (above TN). The gap value
was evaluated at Δ = 14 meV from 1D profiles. (fromRef. [18])and the wave numbers in the other direction are totally unchanged. Thus, we can safely accumulate thespectra with a finite index L. The spectra at T = 40 K,
where the 1D Ni chain can be bare without any magnetic perturbation, shows the original gap value of
14 meV. In contrast, the gap peak merged into the CEF
peaks at 24 meV, which shows a much narrower profile. Although the energy resolution is not sufficient toReferences[1] Haldane F D M 1983 Phys. Lett. 93 464.
[2] Haldane F D M 1983 Phys. Rev. Lett. 50 1153.
[3] Darriet J and Regnault L P 1993 Solid State
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[5] Sachan V, Buttrey D J, Tranquada J M and Shirane G
1994 Phys. Rev. B 49 9658.
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[7] Zheludev A, Tranquada J M, Vogt T and Buttrey D J
1996 Phys. Rev. B 54 6437.
[8] Yokoo T, Zheludev A, Nakamura M and Akimitsu J
35

Research and Development Highlights

MLF Annual Report 2014

1997 Phys. Rev. B 55 11516.
[9] Yokoo T, Raymond S, Zheludev A, Maslov S,
Ressouche E, Zaliznyak I, Erwin R, Nakamura M andAkimitsu J 1998 Phys. Rev. B 58 14424.
[10] Mattheiss L F 1993 Phys. Rev. B 48 4532.
[11] Eisaki H and Uchida S 1995 J. Phys. Chem. Solids 56
1811.
[12] Dagotto E, Riera J, Sandvik A and Moreo A 1996
Phys. Rev. Lett. 76 1731.
[13] Penc K and Shiba H 1995 Phys. Rev. B 52 R715.
[14] Xu G, Aeppli G, Bisher M E, Broholm C, DiTusa J F,
Frost C D, Ito T, Oka K, Paul R L, Takagi H and Treacy

M M J 2000 Science 289 419.
[15] Sasaki T, Yokoo T, Katano S and Akimitsu J 2005 J.
Phys. Soc. Jpn. 74 267.
[16] Itoh S, Yokoo T, Satoh S, Yano S, Kawana D, Suzuki J
and Sato T J 2011 Nucl. Instrum. Methods A 631 90.
[17] Itoh S, Ueno K and Yokoo T 2012 Nucl. Instrum.
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[18] Yokoo T, Itoh S, Ibuka S, Yoshizawa H, Akimitsu J,
Journal of Physics Conf. Ser. 568 (2014) 042035.
[19] Yokoo T, Itoh S, Kawana D, Yoshizawa H and
Akimitsu J 2014 J. Phys. Conf. Ser. 502 012045.

T. Yokoo1,2, S. Itoh1,2, S. Ibuka1,2, Y. Ikeda3, H. Yoshizawa3, and J. Akimitsu4
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3The Institutefor Solid State Physics, The University of Tokyo; 4Physics Deparment, Aoyama-Gakuin University

1

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MLF Annual Report 2014

Research and Development Highlights

Intermultiplet Transitions in SmFe4P12

2. Experimental
Single crystals of SmFe4P12 were grown by the tinflux method using raw materials of 99.9% (3N)-purenaturally occurring Sm, 3N-Fe, 6N-P and 5N-Sn. The dimensions of most crystals were less than 1 mm. Manysmall single crystals of SmFe4P12 were combined for a
total mass of 2.38 g. Inelastic neutron scattering (INS)experiments were conducted by using the time-offlight high resolution chopper spectrometer HRC at
J-PARC.
Usually it is difficult to do INS experiments on Sm
containing materials because of the huge thermalneutron absorption by natural Sm, but, it is possible toreduce the effects of the neutron absorption by using
higher energy neutrons. As shown in Fig. 1, there is atransmission window between the strong 149Sm nuclear resonances which peak at 100 meV and 900 meV.
Therefore, we chose high incident neutron energy of
Ei = 514.1 meV and a chopper frequency of 600 Hz,
where the scattered neutrons also have low absorption

105
Total Cross Section (barns)

1. Introduction
Filled skutterudites RT4X12 (R = rare-earth, T = transition metal, X = pnictogen) have been intensively
studied because they exhibit unusual low temperature
properties, such as heavy fermion (HF) behavior, multipolar ordering and unconventional superconductivity [1]. Among them, SmFe4P12 is reported to be thefirst Sm-based ferromagnetic Kondo-lattice compound
exhibiting a ferromagnetic transition at the Curie temperature 1.6 K [2]. It shows the unconventional HF statewith the large electronic specific-heat coefficient γ =370 mJ/mol K2, which is the second heaviest in Smbased compounds next to SmOs4Sb12 [3, 4]. As is in
the case with SmOs4Sb12, the γ−value of SmFe4P12 also
seems to be robust against magnetic fields.
In general, the energy from the ground J multiplet
to the first excited J multiplet in Sm and Eu compounds
is known to be not large compared to kBT at room
temperature [5]. Therefore, it is necessary to consider
the influence of the excited J multiplet for these compounds. Although it is reported that the local environment surrounding rare-earth ions has little effect on
the energy between the J multiplets split by the spinorbit interaction [6], it may be important to examine
the energy splitting in the Sm-based HF compounds forunderstanding the unusual electronic states of thesematerials.

Sm
104
103
102
Fe
1

P

10

100

1

10

100

1000

Energy (meV)

Figure 1. Energy dependence of the neutron cross sectionsof natural Sm, Fe and P.

cross sections. In this experimental set up, the instrument resolution at zero energy transfer was a full widthat half maximum of 19 meV.
3. Results
Figure 2 shows the INS energy spectra of SmFe4P12
at temperatures of 6.5 K and 280 K [6]. At the low Q
region, one small inelastic peak was observed around80 meV at 6.5 K as denoted by the arrow in Fig. 2(a). The
peak almost disappears at the high Q region, indicating
its magnetic origin. Except for this small peak around80 meV, no clear difference between the data at 6.5 K
and 280 K was seen. If the small peak corresponds tothe intermultiplet transition between the ground J =5/2 multiplet and the excited J = 7/2 multiplet in Sm3+ion, interestingly, the energy level is much lower than
the free Sm3+ ion value ~130 meV and the reported
values in usual trivalent Sm compounds, for example,
131.5 meV in Sm3+ ion doped in LaF3 and 129 meV in
SmPd3. The low energy is comparable with the energy
gap estimated by the bulk magnetic susceptibility of
SmFe4P12. We also confirmed the existence of small
excitation below 100 meV and the absence of excitation around 130 meV at low Q and low temperaturesby a tentative INS experiment with the incident energy
Ei = 300 meV. Furthermore, the observed rapid decreaseof the intensity of the small peak in Fig. 2 with increasing Q agrees with the theoretical inelastic structure factor of Sm3+ [8].
The intermultiplet transitions in many Sm-based
compounds have been studied by INS experiments.
Specifically, significant changes of INS spectra are37

Research and Development Highlights

MLF Annual Report 2014

10×10–3

0.2

6

(b)
0.1

0.0
-50

SmFe4P12

0Energy (meV)

50

–1

0

50

50

6 Å–1 < Q < 10 Å–1

T = 6.5 K
T = 280 K
00Energy (meV)

Ei = 514.1 meV–1

2Å <Q<6Å
2

0.1

0.0
-50

SmFe4P12

Ei = 514.1 meV

4Intensity

Intensity (arb. units)

Intensity

(a)

8

0.2

T = 6.5 K
T = 280 K
100
Energy (meV)

150

200 0

50

100
Energy (meV)

150

200

Figure 2. Energy spectra of neutrons scattered from SmFe4P12 measured with Ei = 514.1 meV at 6.5 K and 280 K for (a) 2 Å–1 < Q < 6 Å–1
and (b) 6 Å–1 < Q < 10 Å–1, where Q is the magnitude of the scattering vector. The arrow denotes the small inelastic peakat 6.5 K. The insets show the data below 50 meV.

reported in intermediate valence compounds such as
Sm1−xYxS [6, 9]. If the valence of Sm ions in SmFe4P12 deviates slightly from trivalent, the J = 0 to J = 1 excitation
around 36 meV for Sm2+, which has the largest inelastic
structure factor in the rare-earth ions, may be expected.
However, no significant difference between the data at
6.5 K and 280 K around 36 meV was observed as shownin the inset of Fig. 2. This is consistent with the resultsof the magnetic susceptibility and the X-ray absorption
spectra [10].
The strong mixing between 4f electrons and conduction electrons, resulting from the characteristic
cage structure in filled skutterudites, might renormalize the spin-orbit transition between the J multiplets in
SmFe4P12. The present study suggests that the contribution of the excited J = 7/2 multiplet should be taken
into account to understand the electronic states in the
Sm-based filled skutterudites.
References[1] H. Sato, H. Sugawara, Y. Aoki and H. Harima,
Handbook of Magnetic Materials, Vol. 18, ed. K. H.

J. Buschow (Elsevier, 2009).
[2] N. Takeda and M. Ishikawa, J. Phys. Condens. Matter
15 L229-L233 (2003).
[3] S. Sanada et al., J. Phys. Soc. Jpn. 74 246-249 (2005).
[4] W. M. Yuhasz et al., Phys. Rev. B 71 104402-1-9(2005).
[5] J. H. Van Vleck, The Theory of Electric and Magnetic
Susceptibilities (Oxford University Press, 1932).
[6] R. Osborn, S. W. Lovesey, A. D. Taylor and E. Balkar,
Handbook of Physics and Chemistry of Rare
Earths, Vol. 19, ed. K. A. Gschneider Jr. and L. Eyring(Elsevier, 1991).
[7] S. Konno et al., J. Phys. Conf. Ser. 592 012029-1-6(2015).
[8] E. Balcar and S. W. Lovesey, Theory of Magnetic
Neutron and Photon Scattering (Clarendon Press,
1989).
[9] P. A. Alekseev et al., Phys. Rev. B 74 035114 -1-13(2006).
[10] M. Mizumaki et al., J. Phys. Soc. Jpn. 76 053706-1-4(2007).

S. Konno1, A. Suzuki1, K. Nihei1, K. Kuwahara1, D. Kawana2, T. Yokoo3, and S. Itoh3
Institute of Applied Beam Science, Ibaraki University; 2The Institute for Solid State Physics, The University of Tokyo; 3Neutron Science
Section, Materials and Life Science Division, J-PARC Center

1

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MLF Annual Report 2014

Research and Development Highlights

Observation of the Inside of a Lithium-ion Battery
by Muonic X-ray
The measurement principle of an elemental analysis
technique with muonic x-ray has been known for over
30 years [1]. Since sufficient flux of negative muons (μ−)
with low energy can now be obtained due to the recent development of the intense pulsed muon source
at J-PARC, several experiments with muonic x-ray havebeen reported since 2008 [2-5]. These experiments are
non-destructive elemental analyses of cultural property [3] or a small amount of rare meteorites [5] with thegreat advantage of high penetrating power and highresolution in depth.
We have applied this non-destructive analysis tolithium-ion batteries, for which it is urgently required to
improve their safety and durability. The key technique isto keep the Li-distribution homogeneous in electrodes
and electrolyte under working conditions; when the
distribution becomes inhomogeneous, the segregated
Li ions change into a needle-shape crystal (dendrite),leading to short circuit of the battery.
As a first step of the Li elemental analysis on thebattery structure, we measured the LiF crystals sandwiched by two sheets of Al foils, in order to make surethat a signal from Li can be obtained through multilayers. As a result, we observed the Li-Kα signal at
18.7 keV [Fig. 1]. This is, to our knowledge, the first datafor detecting the Li-Kα signal by muonic x-ray – Li hassuch a small atomic number that the muon K-α signal
detection requires high resolution in low energy.
We have initiated an elemental analysis on a model
sample consisting of stacked sheets of an uncharged
anode and cathode, separator, which are designed for
a commercial lithium-ion battery, and Al laminatedfilms [Fig. 2], instead of a commercial lithium-ion battery itself with a thick Al outer case. Figure 2 shows an
estimation of the range of μ− in the multi-layered model
sample by a Monte Carlo simulation with SRIM [6].
We have obtained profiles of muonic x-ray with themomentum of μ− (Mμ) at 21.2 MeV/c and 15.7 MeV/c, respectively [Figs. 3 and Figs. 4]. The profile of the cathode[Fig. 3(a)] includes a clear peak of the Al-Lα signal, while
such a peak in the anode is weak [Fig. 4(a)]. The former isnaturally caused by the Al current collector in the cathode sheet, and the latter is thought to be a backgroundsignal from the sample chamber made of Al. It should

Figure 1. The profile obtained for LiF crystals sandwiched by
two sheets of Al foils.

Figure 2. Illustration of the multi-layered sample. The arrows
indicate the range of μ− in the sample.

Figure 3. (a) Muonic x-ray profile with Mμ= 21.2 MeV/c. (b) Enlarged view in the low-energy region below 30 keV.

39

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MLF Annual Report 2014

Figure 5. The ratio of the intensity of signals of μC-Lβ andμC-Lα for the anode and the cathode in the multilayered sample and a graphite.

Figure 4. (a) Muonic x-ray profile with Mμ = 15.7 MeV/c. (b) Enlarged view in the low-energy region below 30 keV.

be noted that both C-Lα and C-Lβ signals are clearly observed in the both profiles at ELα = 13.95 keV and ELβ =18.83 keV. Since the anode consists of graphite and Cu,
the observed result is very reasonable. The cathode, on
the other hand, also includes ~ 5 wt% carbon in order toincrease the electric conductivity. This is the reason why
the signals from C are detected for the cathode sheet.
Since the energy of the C-Lβ (= 18.83 keV) signal is
only 0.13 keV lower than that of the Li-Kα (= 18.70 keV),
we could not separate the two signals in the profile ofthe cathode by the Ge semiconductor detectors withenergy resolution 0.4 keV.
We have obtained muonic x-ray profile on a plate ofgraphite to confirm that the intensity ratio of the C-Lα
signal to that of C-Lβ is intrinsic, that is, 1 : 0.28. In fact,

the ratio in the profile of the anode was found to be
1 : 0.31. However, we determined the ratio as 1 : 0.51 in
the cathode profile [Fig. 5]. If we assume that the ratio of
the intensity of the C-Lα signal to that of C-Lβ does notdepend on conditions, where other elements, including
Li, exist together with C, we could estimate the contribution of the Li-Kα signal to the peak at E ~ 18.8 keV in
the profile for the cathode [Fig. 3(b)].
References[1] H. Daniel et al., Nucl. Instr. Meth. B3 (1984) 65.
[2] M. K. Kubo, K. Ninomiya, et al., J. Radioanal. Nucl.
Chem. 278 (2008) 777.
[3] K. Ninomiya et al., J. Phys. Conf. Ser. 225 (2010)
012040.
[4] K. Ninomiya et al., Bull. Chem. Soc. Jpn. 85 (2012)228㸬
[5] K. Terada et al., Nature Scienti_c Reports 4 (2014)5072㸬
[6] SRIM is a software package for calculating therange of ions in solids and available here; http://
www.srim.org/

I. Umegaki1, H. Nozaki1, K. Ninomiya2, M. K. Kubo3, M. Tampo4, K. Hamada4, N. Kawamura4, Y. Miyake4, H. Yamashige5,
and J. Sugiyama1
1
Toyota Central Research and Development Laboratories, Inc.; 2Osaka University; 3International Christian University; 4Muon Science
Laboratory, High Energy Accelerator Research Organization (KEK); 5Toyota Motor Corporation

40

MLF Annual Report 2014

Research and Development Highlights

Systematic Studies on Muonium Production in Vacuum
from Structured Silica Aerogel
1. Introduction
The goal of this experiment is to systematically study
muonium emission to vacuum from newly developed
silica aerogel with laser-ablated holes. The developmentof muonium emitting material with high efficiency fromsurface muon beams is required for the introduction of an
ultra-slow muon source in the muon g-2/EDM experiment
at MUSE H-line [1]. Such a material would also be desired inother applications that utilize the ultra-slow muon beam.
In the past, two measurements of muonium emissions from silica aerogel were done at TRIUMF before
this experiment [3, 4]. The second measurement at
TRIUMF in 2013 tested the laser-ablated samples andgave an order of magnitude enhancement of the muonium yield. In this study, we tested the newly developed laser-ablated silica aerogel samples by using the
track-back system for decay positrons at the J-PARC
D-line.

developed three new samples with holes. The diameterof holes was about 55 μm. The chosen hole pitch was
285 μm, 185 μm, and 115 μm, respectively. As a reference, we took data with the same sample that was used
in Ref. [2, 4]. Figure 1 shows a schematic representationof the newly developed silica aerogel samples with laser-ablated holes.
3. Experimental method
The experiment used the surface muon beam at
the MUSE D2 area. Sub-surface muons with momentum
23.7 MeV/c were used. The beam momentum is tuned
so that half of the muons are stopped in the target tomaximize muon stopping density at the rear surface ofthe target. A description of the experimental apparatus
is given in Ref. [2].

2. Aerogel samples
The silica aerogel samples were developed in Chiba
university [5]. The laser-ablation processing was doneat the laser-processing facility in RIKEN. In this study, we

4. Results
The time distribution of positrons for the three z
regions are shown in Fig. 2. Signal from muonium in
vacuum observed as event excess over the silica plate
data in the vacuum regions are clearly seen in the time
region t > 2 μs.

Figure 1. Schematic representation of the laser-ablated aerogel sample.

Figure 2. Time distribution of positrons from three z regions
for the Laser-ablated aerogel sample (preliminary
results).

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Research and Development Highlights

MLF Annual Report 2014

By combining the results from the previous
study [2], we confirmed that introducing laser-ablated
holes in silica aerogel increases the muonium yield withindependently-processed samples. The muonium yieldin vacuum for the 115 μm-pitch sample is similar to thereference sample with a lager pitch (300 μm) and holediameter (270 μm). We noticed that the deformation of
the sample was much lower for these samples than of
the reference sample. Flat surface is preferred for better
match to the muonium ionization laser. Therefore, the
new sample would be better suited for the muonium
production target at the ultra-slow muon source.
5. Acknowledgment
The authors are pleased to acknowledge the support from the J-PARC MUSE facility by providing a stablebeam during the experiment. We would like to thankDr. K. Sugioka and his group for their assistance in laser
processing at RIKEN. Our research was supported in partby the MEXT KAKENHI Grant Number 2318005 (Japan),
NSERC Discovery Grant (Canada), and the Center for
Korean J-PARC Users No. NRF-2013K1A3A7A06056592(Korea).
References[1] J-PARC E34 conceptual design report, (2011).
[2] G. Beer et al., KEK-MSL progress report 2013, pp 57(2013).
[3] P. Bakule et al., Prog. Theor. Exp. Phys., 103C01(2013).
[4] G. Beer et al., Prog. Theor. Exp. Phys. 091C01 (2014).
[5] M. Tabata et al., Nucl. Instrum. Meth. A 668, 64(2012).

G. A. Beer1, Y. Fukao6, H. Fujimori7, Y. Ikedo7, K. Ishida8, M. Iwasaki8, S. Kanda8,5,H. Kawai2, N. Kawamura7, R. Kitamura8,5,K. M. Kojima7, S. Lee3, W. Lee3, J. Nakamura7, S. Nishimura5, S. Makimura7, G. M. Marshall10, T. Mibe6, Y. Miyake7,T. Nagatomo9,
Y. Nagashima4, K. Nagumo4, S. Okada8, A. Olin10,1, Y. Oishi8, M. Otani6, N. Saito6,5, K. Shimomura7, P. Strasser7, T. Suzuki4, M. Tabata2,
K. Ueno6, and E. Won3
1
Department of Physics and Astronomy, University of Victoria; 2Department of Physics, Chiba University; 3Department of Physics, Korea
University; 4Department of Physics, Tokyo University of Science; 5Department of Physics, The University of Tokyo; 6Institute of Particle andNuclear Studies, High Energy Accelerator Research Organization (KEK-IPNS); 7Muon Science Laboratory, High Energy Accelerator Research
Organization (KEK-IMSS); 8Advanced Meson Science Laboratory, Nishina Center for Accelerator-Based Science, RIKEN; 9Accelerator
Group, Nishina Center for Accelerator-Based Science, RIKEN; 10TRIUMF

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MLF Annual Report 2014

Research and Development Highlights

Neutron Activation Analysis using Pulsed Neutrons at
J-PARC ANNRI
1. Introduction
Many different analytical methods for multi-elemental analysis have been developed and improved
during the recent decades due to its importance infundamental research and applied technology. In manycases, a nondestructive method is preferred because
the specimen can be reused, as it is, after the measurement. Prompt gamma-ray analysis (PGA) [1] and timeof-flight elemental analysis (TOF), formally known as
neutron resonance capture analysis (NRCA) [2], are nondestructive and multi-element analytical techniques.
Both methods use neutron beams, and measure the
gamma rays produced by neutron capture reactions.
The characteristic energies of the gamma rays emitted
in neutron capture reactions are used as fingerprints fornuclei identification in PGA. By contrast, TOF enables
us to determine the nuclei contained in the sample by
the measuring the energy of the neutron capture resonance. PGA and TOF are similar methods. Then, these
could be replaced by a single measurement. However,PGA and TOF have never been simultaneously applied
for elemental analyses since the gamma-ray detector used is different. We have developed a new analytical technique that combines PGA and TOF by using
an intense pulsed neutron beam at the Japan Proton
Accelerator Research Complex (J-PARC) [3].
Most pure metal samples provide clear peaks on
the PGA and TOF spectra. Thus, these elements are typically easy to measure by PGA and TOF for a single element sample. In contrast, severe peak overlaps in both
PGA and TOF spectra will occur when a mixed sample
is measured. Therefore, the analysis of the mixed samples provides a clear and simple demonstration of theadvantage of the TOF-PGA method. Here, we demonstrate how the TOF-PGA method enables us to extract
reliable information from unresolved peaks in both PGA
and TOF spectra.
2. Experimental
The Accurate Neutron-Nucleus Reaction
Measurement Instrument (ANNRI) has been designed
and developed for PGA, nuclear data measurement,
and nuclear astrophysics [4, 5]. ANNRI is located atbeamline No. 04 at the Materials and Life Science
Experimental Facility (MLF) of J-PARC. MLF is high intensive pulsed neutron facility, which operates at approximately 500 kW proton beam power that will be
increased up to 1 MW in the near future. The germanium detector-array, which is a combination of two
cluster-Ge detectors, eight large coaxial-Ge detectors
and BGO anti-Compton shields surrounding cluster-Geand coaxial Ge detectors, is being installed at the flightpath length of 21.5 m in ANNRI. Each cluster-Ge detector consists of seven individually encapsulated coaxialGe detectors. The absolute photo peak efficiency of thearray for 1.3 MeV of a gamma ray is approximately 3.6%.
3. Results and Discussion
Ag, Au, Cd, Co, and Ta are commonly used as standard samples. In this study, we have measured a mixed
sample that includes these elements. The sample
weights are approximately 13, 5, 23, 1 and 41 mg for
Ag, Au, Co, Cd and Ta, respectively. Figure 1 shows the
PGA and TOF spectra of the mixed sample. All intense
gamma rays from Co overlap ones from other elements in the sample and the background. The neutron

Figure 1. Prompt gamma-ray and time-of-flight spectra. Intense gamma-ray peaks (1) and some of resonance peaks (2) are labeledwith chemical symbols.

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Research and Development Highlights

MLF Annual Report 2014

Figure 2. TOF-PGA spectrum analysis by gating on the PGA peaks.

resonance peak of approximately 130 eV of Co has serious overlap with that of Ta (and Ag) because the widthof the Co peak is broad. Consequently, time-consuming
and very careful peak shape analysis for unresolved
peaks is required to obtain accurate results for Co byeither PGA or TOF in the present experiment. It is quite
likely that neither PGA nor TOF can obtain accurate results in some cases, especially if a sample contains a
number of elements.
Figure 2 shows the TOF-PGA spectrum analysisof the mixed sample by gating on the TOF peaks. The
gamma-ray peaks that are used for making the gatedspectra seen in Figure 2 contain the γ rays not only fromCo but also from the other elements. Most of overlapping gamma-ray events appear in different points on
the gated TOF spectrum because the resonance peakenergies of Co are different from most of these of Cd, Ta
etc. As a result, the TOF-PGA method allows us to eliminate or at least greatly suppress the contributions of theother elements and the background in the Co peak, andcan accurately quantify Co even with the presence of
these elements.

TOF-PGA method will be an irreplaceable tool for
research in many fields because it makes it possible toobtain reliable and valid results.
4. Acknowledgement
This work was supported in part by Grants-in-Aid
for Scientific Research (25246038)
References[1] M. P. Failey, D. L. Anderson, W. H. Zoller, G. E. Gordon,
R. M. Lindstrom, Anal. Chem. 1979, 51, 2209-2221.
[2] H. Postma, M. Blaauw, P. Bode, P. Mutti, F. Corvi, P. J.
Siegler, Radioanal. Nucl. Chem. 2001, 248, 115-120.
[3] Y. Toh, M. Ebihara, A. Kimura, S. Nakamura, H. Harada,
K. Y. Hara, M. Koizumi, F. Kitatani, K. Furutaka, Anal.
Chem. 2014, 86, 12030-12036.
[4] M. Igashira, Y. Kiyanagi, M. Oshima, Nucl. Instrum.
Methods Phys. Res., Sect. A 2009, 600, 332-334.
[5] H. Harada et al., J. Korean Phys. Soc. 2011, 59,
1547-1552.

Y. Toh1, M. Ebihara2, M. Huang1, A. Kimura1, and S. Nakamura1 on behalf of the ANNRI collaboration
1Nuclear Science and Engineering Center, Japan Atomic Energy Agency; 2Graduate School of Science and Engineering, Tokyo Metropolitan
University

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MLF Annual Report 2014

Research and Development Highlights

Neutron Reflectivity Measurement for Study of Water
Permeability of Anticorrosive Ultrathin Film
1. Introduction
Maintaining and repairing the structural integrity, appearance, and functional properties of metals,
alloys or other structural materials is a matter of immense concern in our daily lives. Corrosion of metals
and alloys is often regarded as a major factor in theseissues. Therefore, various technologies, including chromate passivation, electrochemical plating, anodizing,
and coating/painting, have been used to resolve those
problems [1]. However, with the rapid advance of (nano)science and technology and serious concerns over pollution caused by heavy metals used in major existing
technologies, it is becoming of paramount importanceto find alternative ways to protect modern (nano)devices from corrosive hazards. Within this context, we havebeen exploring a biomimetic anticorrosion ultrathin

Figure 1. Chemical structure of poly(dopamine methacrylamide-co-alkyl methacrylate), poly(DOMA-co-AMA).

Figure 2. Images of half-coated metal/alloy plates embedded
in resin after immersion in corrosive salt-water solution (3.5 wt.% in water) for several days. Left and rightside shows uncoated and coated area, respectively.

polymer coating produced through a versatile, ecofriendly and easy process. Specifically, poly(dopamine
methacrylamide-co-alkyl methacrylate), poly(DOMAco-AMA) (Fig. 1) exhibited a great potential as a highperformance anticorrosive coating. Here dopamine,
which is a key component of the adhesive secretion of
the blue mussel, was utilized as an adhesive moiety towards a variety of substrates. As expected, the obtainedpoly(DOMA-co-AMA) demonstrated excellent anticorrosion property on variety of metals and alloys (Fig. 2).
Most importantly, thermal treatment of the as-spun ultrathin film drastically improved anticorrosion property
for longer duration in sharp contrast with the film without thermal treatment that gets damaged by corrosion
just after several days. To address the question about
how thermal treatment affects preventive ability ofthe polymer film, we evaluated water penetration into
the polymer thin film using neutron reflectivity (NR,
SOFIA@BL-16), which is one of the most depth-sensitivetechniques [2, 3].
2. Experimental
Tetrahydrofuran (THF) solution of poly(DOMA-coAMA) was spun on a silicon block. If the density profile of thin-film is examined along normal direction to
the surface only in air, the X-ray reflectivity should begood enough. However, we focused on density profilesof the coating layer in contact with liquids. The density profiles of the film in air and in contact with water
were examined by NR measurements using horizontal
type neutron reflectometer SOFIA at the Materials andLife Science Experimental Facility (MLF). A glass reservoir filled with liquid was mounted onto the film. The
measurements were conducted in air, and then in purified and degassed deuterated water (D2O). Prior tothe measurements in D2O, the film was aged in D2O for
2 h, which was apparently enough to cause a structuralchange in the film. A beam of neutrons with a wavelength (λ) that ranged from 0.25 to 0.88 nm at a resolution of 3% was guided into the specimen from thesilicon side. Details of our experimental setup were described elsewhere [4, 5]. The reflectivity was calculatedon the basis of the model (b/V) profile along the depth
direction by means of Parratt 32 software, a freewareprogram from the Hahn-Meitner Institute.

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Research and Development Highlights

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3. Discussion
Figures 3a and 3c show the reflectivity curves as afunction of the scattering vector (q = (4π/λ)sinθ, where
λ and θ are the wave length and the incident angles of
the neutron beams, respectively) for as-spun and annealed poly(DOMA-co-AMA) films under air and deuterated water (D2O). For clarity, the data set for thefilm in D2O is offset by three orders of magnitude. The
open symbols denote the experimental data, and thesolid curves were fit curves calculated from the scattering length density (b/V) profiles in Fig. 3b and 3d.
To understand the role of thermal treatment and theimportance of the catechol units for high anticorrosion
efficiency, only interfacial regions are shown. Since thesolid curves in Fig. 3a and 3c are in good agreementwith the experimental data, it is most likely that themodel (b/V) profiles depicted in Fig. 3b and 3d would
reflect the density profiles of the films. The (b/V) values
for silicon (Si), native oxide layer (SiOx) and D2O used inthese calculations were 2.21 × 10−4, 4.18 × 10−4, and 6.62
× 10−4 nm−2, respectively. In both cases, when measured
under air, the (b/V) values were constant over the entire
region of the film thickness with ca. 150 nm, except for
the interface with the Si substrate. This indicates that aslightly dense layer formed with ca. 5 nm in thickness
adjacent to the substrate, although the density of theupper region was identical to the polymer bulk. Since
this phenomenon was not observed for spin-coatedpoly(methyl methacrylate) (PMMA) film, [4] it is more
likely that the catechol moiety stimulated anchoring of
the polymer chains to the substrate and resulted in aslightly dense layer at the interface. In the case of measurement under water for non-annealed film, the (b/V)
value was drastically changed (Fig. 3b). The magnitude
was slightly higher than that in air, and increased substantially at the substrate interface. This indicates thatthe adsorbed D2O molecules (with high (b/V) value)
reached the substrate and enriched it. Similar behavior
has been reported for PMMA spin-coated film, in whichtiny channels were generated during solvent evaporation, and within several hours the thin film was swelledby the penetrated water molecules [5]. Surprisingly, theannealing process overcame this shortcoming and significantly improved the barrier ability against foreign
molecules. Thus in the case of annealed film, D2O could
not penetrate the substrate even after 2 hours of immersion in D2O, which otherwise would be enoughtime to cause swelling by the water molecules (Fig. 3d).
These results suggest that the annealing aids the closing of the tiny channels and makes the polymer chain46

arrangements more uniform, leading to prevention offoreign molecules. Therefore, we conclude that a combination of formation of a ca. 5 nm dense layer adjacentto the substrate and thermally cured sub-micron layer
above this dense layer completely inhibits the penetration of foreign molecules and exhibits high anticorrosion property (Fig. 4).

Figure 3. Neutron reflectivity for (a) as-spun and (c) annealed
films in air and water. Open symbols depict experimental data, and solid lines represent the reflectivity
calculated on the basis of the scattering length density(b/V) profiles shown in (b, d). For clarity, the values inpanel (a, c) are offset from one another.

Figure 4. Schematic illustration of difference between as-spunand annealed film determined by neutron reflectivity
measurement.

In conclusion, we have developed a simple andpractical coating method for anti-corrosion of versatile
metals and alloys inspired by an underwater bio-adhesion [1]. On the basis of NR technique, we observedthat spin-coated copolymers enabled the formation ofa dense nanolayer adjacent to the metal surface, which
normally does not occur with conventional poly(alkyl
methacrylate)s. This happened by strong binding affinity of the catechol unit towards metal/alloy substrates,
resulting in a spontaneous condensation of the polymer chains at the metal interface. Additionally, theMLF Annual Report 2014

annealing process was found to be essential to improve
the protecting ability against corrosive molecules, due
to the formation of defect-free coating.
References[1] D. Payra, M. Naito, Y. Fujii, N. L. Yamada, S. Hiromoto,A. Singh, RSC Adv., 5, 15977 (2015).
[2] N. L. Yamada, N. Torikai, K. Mitamura, H. Sagehashi,
S. Sato, H. Seto, T. Sugita, S. Goko, M. Furusaka, T.
Oda, M. Hino, T. Fujiwara, H. Takahashi, A. Takahara,

Research and Development Highlights

Eur. Phys. J. Plus, 126, 108 (2011).
[3] K. Mitamura, N. L. Yamada, H. Sagehashi, N. Torikai,
H. Arita, M. Terada, M. Kobayashi, S. Sato, H. Seto,
S. Goko, M. Furusaka, T. Oda, M. Hino, H. Jinnai, A.
Takahara, Polym. J., 45, 100. (2013).
[4] K. Tanaka, Y. Fujii, H. Atarashi, K. Akabori, M. Hino, T.
Nagamura, Langmuir, 24, 296 (2008).
[5] H. Atarashi, T. Hirai, K. Hori, M. Hino, H. Morita, T.
Serizawa, K. Tanaka, RSC Adv., 3, 3516 (2013).

M. Naito1, Y. Fujii2, D. Payra1, and N. L. Yamada3
Research Center for Strategic Materials, Structural Materials Unit, National Institute for Materials Science (NIMS); 2Advanced Key
Technologies Division, Polymer Materials Unit, National Institute for Materials Science; 3Neutron Science Division, Institute of Materials
Structure Science, High Energy Acceleration Research Organization

1

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Research and Development Highlights

MLF Annual Report 2014

Measurement of Neutron Spatial Brightness from
Coupled and Decoupled Para-hydrogen Moderators
Introduction
A moderator’s neutron spatial brightness is one of
the most important pieces of data needed for its proper
design.
Especially, after it was reported that a liquid parahydrogen moderator had an eccentric spatial brightness
in the simulation [1]. The measurement of the spatial
brightness is necessary for the Japanese Spallation
Neutron Source (JSNS) Group to validate the neutronic
design of JSNS at J-PARC. On the other hand, because
the European Spallation Source (ESS) Group proposesa flat liquid hydrogen coupled moderator in the ESS
design, they require the special brightness data fromthe coupled liquid hydrogen needed for the coupled
spatial distribution. Therefore, the JSNS Group and the
ESS Group collaborated to measure the neutron spatial
brightness for the moderators at J-PARC.
Measurements and Results
The nGEM detector [2], which was a gaseous ionization chamber using boron files, prepared for theneutron imaging experiment at BL22, was used for themeasurement. Two measurements were done at BL10for the decoupled moderator and at BL04 for the coupled moderator. At BL10, the detector was located at
13 m and a tiny collimator (3.1 × 3.1 mm) in the rotarycollimator at 8.0 m was used. At BL04, the detector was
located at 28.5 m and a pinhole Cd plate with a hole of
3 mm in diameter was placed at 21.5 m.
Figure 1 shows the neutron spatial brightness
around 5 meV from the decoupled moderator (BL10).
The figure on the left shows the measurement result
and the one on the right depicts the simulation. The
simulation was done by PHITS [3] calculation with theengineering model of JSNS [4]. It was found that the
distributions of the two sets of data were very similar
with the largest intensities at the center. Also, an aluminum tube in the moderator was observed (the twovertical lines near the center).
Figure 2 shows the neutron spatial brightness
around 5 meV from the coupled moderator (BL04). In
the same way as in Fig. 1, the figure on the left shows
the measurement result and the one on the right

Figure 1. Neutron spatial distribution from the decoupled moderator (BL10) Left: measurement; right: simulation.

Figure 2. Neutron spatial distribution from the decoupled moderator (BL04) Left: measurement; right: simulation.

depicts the simulation. It was found that the distributions of the two sets of data were very similar and thelargest intensities were observed near the target (upperside) and far from it (lower side).
Summary
The particular spatial brightness from the coupledmoderator is of great interest to us and it is very important to measure these data for the moderator in ahigh-power spallation neutron source. These results
validated the JSNS neutronic design. And they would
be also very helpful for the ESS design.
References[1] T. Kai et al., Nucl. Instr. Meth. A, 523 398 (2004).
[2] S. Uno et al., Physica Procedia, 26, 142 (2012).
[3] T. Sato, J. Nucl. Sci. Technol., 50, 913 (2013).
[4] M. Harada et al., Prog. Nucl. Sci. Technol., 2, 872(2011).

M. Harada1, M. Teshigawara1, M. Ooi1, K. Esben2, and L. Zanini2
Neutron Source Section, Materials and Life Science Division, J-PARC Center JAEA; 2European Spallatin Source ESS AB

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MLF Annual Report 2014

Research and Development Highlights

Dynamic Structures of Superionic Conductors of
MAg4I5 (M = K, Rb) by Inelastic Neutron Scattering
1. Introduction
RbAg4I5 and KAg4I5 are well known as superionic
conductors [1, 2]. In particular, RbAg4I5 has a superionic phase in a wide temperature range from −155 to
228°C [1] and remains a solid electrolyte even at ambient temperature. In the superionic phase of RbAg4I5
and KAg4I5, the Ag ions migrate through the sublattice
formed by the I and Rb (or K) ions, as shown in Fig. 1 [3].
The ionic conductivity of RbAg4I5 (σ = 0.21(6) Ω−1cm−1)
is approximately three times higher than that of KAg4I5(σ = 0.08(5) Ω−1cm−1) at ambient temperature [2]. It was
proposed that the Rb ion, whose radius is larger thanthat of the K ion, causes a lattice expansion, which contributes to easier Ag diffusion in RbAg4I5 [2]. Shapiro et
al. reported the energy dependence of inelastic neutron
scattering for single crystalline RbAg4I5 at Q = (0, 5.7, 5.7),
and the low-energy excitation peak was found at aroundE = 2.5 meV [4], which is consistent with the results of polarized Raman scattering [5]. This low-energy excitation
is presumed to be caused by local vibrations of Ag ions
within an immobile cage formed by I ions [4, 5]. On theother hand, KAg4I5 has not been studied using inelastic
neutron scattering and even Raman scattering.
In the present study, inelastic neutron scattering
measurements were carried out for RbAg4I5 and KAg4I5
at the BL14 beamline (AMATERAS: Cold–Neutron Disc–
Chopper Spectrometer) to investigate the difference inthe low-energy excitations in the two materials.

Figure 1. Crystal structure of superionic phase of RbAg4I5 andKAg4I5. Blue, pink, and purple spheres exhibit Ag, Rb(or K), and I ions, respectively.

2. Inelastic Neutron Scattering
The sample of RbAg4I5 was prepared from powder
samples of pure RbI and AgI by mixing them in a quartz
tube under vacuum at 1073 K above their melting
points, and then cooling to solidify the mix into a bulk
sample. After this process, the sample was annealed at
510 K for 48 hours and powdered at room temperature,
just before the experiments. Although the sample of
KAg4I5 was prepared in the same manner as RbAg4I5, theanneal temperature for KAg4I5 was 500 K which was thesame temperature applied in the experiment in reference [2]. Each sample was placed in an Al-foil cell, whichweighed 20 g. This Al-foil cell was set in the Al standard
cell which was architected for the inelastic neutron
scattering measurements. The inside of the Al standard
cell was filled with He gas. The inelastic neutron scattering measurements were carried out with time-of-flighttechnique [6]. AMATERAS covers a scattering angle of 5°~ 112° horizontally and −16° ~ 22° vertically. For an easy
access to the dynamics in different time scales, multi-Ei
technique [7] was applied, where the monochromating chopper operating at 150 Hz, 6 times faster than theneutron pulse emerging at 25 Hz, and the band chopper at 25 Hz yielded incident energies (Ei’s) of 94.3, 23.7,
10.5 and 5.9 meV simultaneously with energy resolutions of 8.4, 1.1, 0.4 and 0.15 meV for elastic scattering,
respectively. In the case of RbAg4I5, the sample temperature was controlled by using a cryo-furnace within
a wide temperature range from 10 K to 348 K. Since
KAg4I5 decomposes to AgI and K2AgI3 below 311 K [8],the sample temperature was kept at around 348 K during the sample setup and the measurement for KAg4I5
was carried out only at 348 K. We confirmed that the
sample was not decomposed by confirming that the
profile of the elastic spectrum was maintained in themeasurement process.
3. Results and Discussion
The energy dependence of the dynamic structure
factor S(Q,E) for RbAg4I5 at T = 135 K and several Q points
are shown in Fig. 2. Although no characteristic peak isobserved at small Q (= 1.35 Å−1), a single low-energy
excitation peak is observed at around E = 1.5 meV andQ = 1.73 Å−1. In the middle Q region ( > 2 Å−1), an additional low-energy excitation peak is clearly observed ataround E = 2.2 meV.
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Research and Development Highlights

MLF Annual Report 2014

Figure 2. Energy dependence of dynamic structure factors,
S(Q, E), sliced at several Q points for RbAg4I5 at T =135 K with Ei = 5.9 meV.

Figure 3 shows the energy dependence of normalized S(Q,E) for the superionic phases of RbAg4I5 andKAg4I5 at T = 348 K. Å−1. S(Q,E) for KAg4I5 has a single
peak at around E = 1.7 meV and Q = 1.73, and the peakheight is lower than that for RbAg4I5. An additional peakis observed in the vicinity of E = 2.4 meV and Q = 1.94 Å−1
for KAg4I5 which grows with increasing Q. Although
the peak positions are the same for the two materials,
the peak intensities for RbAg4I5 are larger than thosefor KAg4I5 at all Q, indicating that the local vibrationalmodes of Ag ions are easily excited in RbAg4I5 in comparison with KAg4I5, which would relate to the difference in ionic conductivity between the two materials.
References[1] B. B. Owens and G. R. Argue, Science, 157 308 (1967).
[2] S. Hull, D. A. Keen, D. S. Sivia and P. Berastegui, J.
Solid State Chem., 165 363 (2002).
[3] S. Geller, Science, 157 310 (1967).
[4] S. M. Shapiro, D. Semmingsen and M. B. Salamon,
Proc. Int. Conf. on Lattice Dynamics, 538 (1977).

Figure 3. Energy dependence of normalized dynamic structure factors for RbAg4I5 and KAg4I5 at 348 K. These
data are corrected by Bose factor, <n+1> = exp(ħω/kBT) / (exp(ħω/kBT) – 1) and are offset in vertical direction for clarify.

[5] D. Gallagher and M. V. Klein, J. Phys. C: Solid State
Phys., 9 L687 (1976).
[6] K. Nakajima, S. Ohira-Kawamura, T. Kikuchi, M.
Nakamura, R. Kajimoto, Y. Inamura, N. Takahashi,
K. Aizawa, K. Suzuya, K. Shibata, T. Nakatani, K.
Soyama, R. Maruyama, H. Tanaka, W. Kambara,
T. Iwahashi, Y. Itoh, T. Osakabe, S. Wakimoto, K.
Kakurai, F. Maekawa, M. Harada, K. Oikawa, R. E.
Lechner, F. Mezei and M. Arai, J. Phys. Soc. Jpn., 80
SB028 (2011).
[7] M. Nakamura, R. Kajimoto, Y. Inamura, F. Mizuno,
M. Fujita, T. Yokoo and M. Arai, J. Phys. Soc. Jpn., 78093002 (2009).
[8] J. N. Bradley and P. D. Greene, Trans. Faraday Soc., 63
424 (1967).
[9] K. Shibata and S. Hoshino, J. Phys. Soc. Jpn., 54 3671
(1985).

S. Tahara1,2, Y. Kawakita3, M. Nakamura3, H. Shimakura4, T. Kikuchi3, Y. Inamura3, K. Nakajima3, S. Ohira-Kawamura3, T. Sunakawa1,
and T. Fukami1
1
Department of Physics and Earth Sciences, Faculty of Science, University of the Ryukyus; 2Research and Utilization Division, Japan
Synchrotron Radiation Research Institution (JASRI/SPring-8); 3Neutron Science Section, Materials and Life Science Division, J-PARC Center;
4Faculty of Pharmacy, Niigata University of Pharmacy and Applied Life Sciences

50

MLF Annual Report 2014

Research and Development Highlights

Progress in the Dynamic Nuclear Polarization on POLANO
1. Introduction
Polarized neutron scattering is a useful method
for conducting studies in materials science. One of theways to polarize neutrons is by using a polarized proton
target (PPT). As neutron-proton scattering length of thetriplet channel is much smaller than that of the singlet
channel [1], the neutron beam transmitted through a
PPT gets polarized.
A brute-force way to polarize sufficient number ofprotons in the target is by applying a strong external
magnetic field to it and cooling it down to a low temperature. However, even if we cool it down to 1 K andapply an external magnetic field of 5 T to it, the thermal equilibrium Boltzmann polarization of the protons
is still less than 1% and the target cannot be used as apractical neutron polarizer.
To highly polarize proton spins, we can use thedynamic nuclear polarization (DNP) method. In theabove mentioned situation, although the polarizationof protons is less than 1%, that of unpaired-electrons
is nearly equal to unity since the magnetic moment of
the electron is much larger than that of the proton. The
DNP method exploits the microwave-irradiation-driven transfer of polarization from unpaired-electrons toprotons. To test the enhancement of the proton polarization by this method for several target materials that
contain protons and unpaired-electrons and estimate
their performance as neutron polarizers for POLANO,
we are preparing instruments for DNP of proton spins.

using a mechanical tuner. The output power is typically 20 W and depends on the output frequency.
To control the output power, we prepared a variableattenuator (Keycom, AT-8-20). Most of the microwave
power through the attenuator was directed at the cryostat using standard F-band rectangular waveguides.
A small part of it was coupled off by a directional coupler (Keycom, DC-8-10) to estimate the power and measure the frequency fed to the cryostat. The spectrumof the microwave that was coupled off by the coupler
was measured using a spectrum analyzer (Agilent,
EXA N9010A) and a harmonic mixer (OML, M06HWD).
Figure 1 depicts the measured spectrum, which clearlyshows that a microwave with a frequency of 140 GHz
had been generated.

2. Instruments
To cool down a target and apply an external magnetic field to it, we use the cryostat that was used by
Crabb and coworkers [2]. The 4He evaporation refrigerator can cool the target down to 1 K and the split coilsuperconducting magnet can apply the magnetic fieldof 5 T to it.
To measure the proton polarization, we prepared
instruments, which are used in studies of continuous
wave nuclear magnetic resonance (CW NMR) spectroscopy. As reported in the MLF Annual Report 2013 [3],we measured successfully the signal of a Teflon sheet,
which contains fluorine nucleus whose magnetic moment is 6% smaller than that of a proton.
To irradiate microwave to a target, we prepared
an extended interaction oscillator (Communication &Power Industries, VKT 2438P). The output frequency
can be controlled from 138.5 GHz to 141.5 GHz by

3. Test Sample
To test the system, we prepared a TEMPO(2,2,6,6-tetra-methyl-piperidine-1-oxyl), which contains
unpaired-electrons, doped low-density polyethylene
film, which contains protons.
First, we heated the polyethylene film using a drying oven (Sanyo, MOV-202). 1.888 g of polyethylene
film (Sanipak Company of Japan, L-43) was placed ona plate made of soda-lime glass and inserted into theoven. The temperature was kept at 100 °C for 1 hour. We
then set the setting temperature to a room level andwaited for 2 hours.
Next, we took the film out of the oven and put it
into a vacuum chamber (As One, VCP-15L) for 1 day. The
pressure inside the chamber was 0.4 atm.
Finally, we doped TEMPO (Sigma-Aldrich, 214000)
into the film. We took the film out of the vacuum chamber and put it together with 10 mg of TEMPO powder

Power level (dBm)

0
‐10
‐20
‐30
‐40
‐50
139.9

139.95140140.05Microwave Frequency (GHz)

140.1

Figure 1. A spectrum of microwave through a variable attenuator and a directional coupler.

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MLF Annual Report 2014

into a sealed bottle made of soda-lime glass. We placed
the bottle into the drying oven and kept the insidetemperature at 80 °C for 1 day. We then set the setting
temperature to a room level and waited for 2 hours. To
prevent TEMPO from sublimating from the film, we took
it out of the sealed bottle and put it into a cryopreserving container (Cryo One, SR-31).
If all the amount of TEMPO had been uniformly
absorbed into the film, the spin density would be 2 ×
1019 spins / cc. To estimate how much amount of TEMPO
was doped into the film, we measured its electron spinresonance (ESR) spectrum. We cut off a small piece ofthe film and put it into the microwave cavity of an ESR
spectrometer (JEOL, TE200). By scanning the external
magnetic field applied to the cavity, we observed aclear ESR spectrum shown in Figure 2. Using calibration
data and this spectrum, we estimated that about half of
the TEMPO was absorbed into the film.
4. Plan
We can now irradiate a frequency and power tunable microwave to the target, apply 5 T external magnetic field and cool it down to 1 K. By comparing the
CW NMR spectrums with and without microwave irradiation, we are going to estimate the proton polarization
enhanced by the DNP method.

332

334

336
Magnetic field (mT)

338

Figure 2. The ESR spectrum of the prepared test sample. The
applied microwave frequency was 9.43408 GHz.

Acknowledgement
We thank Takayuki Kumada (JAEA) for the cooperation in measuring the electron spin resonance spectrum of the sample.
References[1] H. A. Bethe and P. Morrison, Elementary Nuclear
Theory (Wiley, 1956).
[2] D. G. Crabb, C. B. Higley, A. D. Krisch, R. S. Raymond,
T. Roser, J. A. Stewart, and G. R. Court, Phys. Rev.
Lett. 64, 2627 (1990).
[3] K. Taketani, S. Ishimoto, S. Itoh, K. Iwasa, K. Ohoyama,
S. Suzuki and T. Yokoo, MLF Annual Report 2013.

K. Taketani1,2, T. Yokoo1,2, Y. Nambu3, S. Itoh1,2, S. Ishimoto4, S. Suzuki4, and T. Otomo1,2
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3Institute forMaterials Research, Tohoku University; 4Institute of Particle and Nuclear Studies, KEK

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Research and Development Highlights

3

He Neutron Spin Filter for POLANO

1. Introduction
A 3He neutron spin filter (NSF) is one of the essential devices in POLANO for polarization of the incident
neutron beam. It is required to be operated in-situ toprovide a stable neutron polarization, and the spin-exchange optical pumping (SEOP) method is employed
to polarize the 3He nuclei. Since there is limited space
to accommodate the 3He NSF, we designed a compact
system that fits well between the disk choppers andthe sample chamber [1]. It is now under development
and will be installed as soon as POLANO gets the firstneutron beam in 2016. The first 3He NSF in POLANO will
cover a neutron beam diameter of 50 mm with neutronenergy up to 100 meV.

3.5 atm, and the effective 3He thickness will range from12 to 35 atm-cm for various measurements.
(2) Homogeneous magnetic field
A solenoid and compensation coils at both solenoid
edges with Permalloy magnetic shield were designed,
and a prototype magnet was constructed (Fig. 2). The
neutrons are polarized in the axial direction in the 3He
NSF, and the spins are rotated adiabatically in the transverse direction by the magnetic guide field [2]. The
compensation coils will be optimized in accordancewith the guide field.

2. R&D on 3He NSF for POLANO
A schematic view of the 3He NSF in POLANO isshown in Fig. 1. The necessary elements for in-situ polarized 3He neutron spin filters are (1) a 3He cell, (2) ahomogeneous magnetic field with neutron guidefields, (3) a high-power laser with optical components
for the optical pumping of Rb, (4) a heater to achieve
the appropriate number densities of K and Rb, and (5)adiabatic fast passage (AFP) spin flipping of polarized
3
He.

Figure 2. Magnetically shielded solenoid to produce a homogeneous field for 3He NSF. The diameter of thesolenoid is 20 cm and the length - 30 cm. Additional magnetic shields will be added to the both endsof the solenoid.

Figure 1. A schematic view of the 3He NSF in POLANO. All theessential elements are packed in a laser shield box
with a size of 60 cm by 60 cm by 25 cm.

(1) 3He cell
We will prepare cylindrical cells made of GE180 aluminosilicate glass with a dimeter of 60 mm and a lengthof 60 to 100 mm. The cells will be filled with 3He at 2.0 to(3) Laser and optical components
A laser diode array with an output power of 100 W
with a chirped volume Bragg (holographic) grating(VBG or VHG) emits a spectrally narrowed 795 nm light(Rb D1 line) for the optical pumping of Rb (Fig. 3). A
quarter waveplate converts the linear polarization into
circular polarization. The waveplate can be remotely
rotated by +/−90 degrees to change the left and rightstates depending on the AFP spin flipping of 3He. The
laser optical apparatus is shown in Fig. 4.
(4) Heater
In SEOP, hot air blowers (compressed air blowers)
are commonly used to keep 3He cells at an elevated53Research and Development Highlights

MLF Annual Report 2014

requires heat insulation around itself for safety. Dueto the limited available space, we have decided not to
use a hot air blower but a thin electric heater made ofpolyimide films and NiCr strips, which is attached to theouter surface of an aluminum oven for a 3He cell. The
NiCr strips will be specially designed in order to minimize the magnetic field interference.

Figure 3. Laser spectra from the 100 W laser diode array(LDA) with and without the chirped volume Bragg
grating (C-VBG). Not only is the spectrum narrowed,
but the peak intensity is also much higher with theuse of the C-VBG.

(5) AFP 3He spin flipper
In almost all measurements with polarized neutrons, neutron spin flipping is a must for cancelling out
any systematic uncertainties. We demonstrated successfully a compact AFP spin flipper for polarized 3Hewith an RF coil positioned inside an aluminum oven [3].
The 3He spins can be flipped within a half second, andthe polarization loss was less than 4 × 10−4 in one spin
flip. Such an AFP spin flipper will be redesigned to fit
the 3He cells described in (1).
3. Safety and future upgrading
The controllers for the in-situ polarized 3He NSF
system are equipped with various safety mechanisms
such as interlocks for the laser and the heater to meet
the J-PARC safety standards. The 3He NSF system will beready for operation by the first day of POLANO’s operation and the goal is to upgrade it continuously to widen
the beam diameter and improve the 3He polarization.

Figure 4. A picture showing the laser optical apparatus, a laser diode array (LDA), a chirped volume Bragg grating (C-VBG), and a quarter waveplate.

temperature because they do not interfere with the homogeneous magnetic field while conventional electricheaters produce unnecessary magnetic fields. However,a hot air blower occupies a fair amount of space andReferences[1] T. Yokoo et. al., “BL23 Polarized Neutron Scattering
Spectrometer POLANO,” in this report.
[2] K. Ohoyama et. al., “Estimation of Magnetic Field
Distribution for Polarized Neutron Experiments,” inthis report.
[3] T. Ino et al., “A compact SEOP 3He neutron spin filter with AFP NMR,” J. Phys.: Conf. Ser. 340, 012006(2012).

T. Ino1,2, M. Ohkawara3, K. Ohoyama4, T. Yokoo1,2, S. Itoh1,2, H. Kira5, H. Hayashida5, K. Sakai6,7, T. Oku6, and K. Kakurai8
Institute of Materials Structure Science, KEK; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center; 3Institute forMaterials Research, Tohoku University; 4Ibaraki University; 5CROSS-Tokai; 6Technology Development Science Section, Materials and Life
Science Division, J-PARC Center; 7Neutron Source Section, Materials and Life Science Division, J-PARC Center; 8Quantum Beam Science
Directorate, JAEA

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Research and Development Highlights

Estimation of Magnetic Field Distribution for Polarized
Neutron Experiments
1. Introduction
A polarization analysis neutron spectrometer,
POLANO, has been constructed at beam line 23 (BL23)
in the second experimental hall of the Materials and Life
Science Experimental Facility (MLF) at the Japan Proton
Accelerator Research Complex (J-PARC) [1, 2].
Since the careful control of the magnetic fields
around the beam is very important for performing precise polarized neutron experiments, magnetic devices,such as guide magnets, Helmholtz coils, and so on, will
be used. However, the optimization of magnetic devices
during beam-times is almost impossible in pulsed neutron spectrometers. Thus, the optimization of magnetic
fields by calculations and off-beam tests is required.
Based on the estimation of magnetic field distributions
by the finite element method, we succeeded in findingalignments of magnetic devices which can provide satisfactory high neutron polarization in the energy range ofup to 100 meV. This report explains the calculation method of transportation of the polarization and its results.
2. Calculation of polarization
To optimize magnetic field distributions, we estimate the change of neutron polarization between thepolarizer and the supermirror analyzer. For BL23, a cylindrical 3He spin filter polarized by the on-beam spin
exchange optical pumping (SEOP) technique will be
used as a polarizer. When neutrons with finite velocity enter a magnetic field, the neutron spin rotates by
Larmor precession. The final spin wave function ψf by
Larmor precession can be represented using the initial
spin wave function ψi as,ψf = exp −i

S n 2ωl
ħ υ

ψi

Pn =

Sx Bx + Sy By + Sz Bz
S B

(3)

Thus, when the magnetic field distribution with an interval of l is provided, the value of Pn at each point canbe estimated.
The calculations of the magnetic field distribution were done using the finite element method program ANSYS in SR16000 supercomputing resources at
the Center for Computational Materials Science of theInstitute for Materials Research, Tohoku University. For
these calculations, the z-axis is defined to be parallelto the beam direction, the y-axis is in the vertical direction, and the x-axis is perpendicular to the y-and z-axes.
Since the magnetic field at the 3He spin filter is parallelto the beam direction, the initial neutron spin is parallelto the z-axis. We assumed the initial neutron polarization at the spin filter to be Pn = 1.
3. Basic alignment of magnetic devices for BL23
Figure 1 shows the basic alignment of the magnetic field devices for BL23. Shown from left to right, are asolenoid coil, a guide coil with a width of 3 cm, squareshape vertical guide magnet with pillars of permanent
ferrite magnets, a Helmholtz coil with additional threecoils which generate horizontal magnetic fields, a guidemagnet with fan-shape with neodymium magnets, anda supermirror analyzer. The magnetic housing for thesupermirror analyzer generates strong magnetic fields
to the mirror; the magnetic field at the center of the
housing is set to about 400 G, when the magnetic mirror is not installed.

(1)Here, ω, l, and υ are Larmor frequency, the length of
the flight path under the magnetic field, and neutron
velocity, respectively. S is the neutron spin and n is theunit vector of the magnetic field, B. The average value ofeach spin component for ψf is obtained as

Sα =

ħ *
ψ σα ψf (α = x, y, z)
2 f

(2)

where σα is the Pauli matrix for α-component. From theaverage spin components, the neutron polarization, Pn,of the final state can be defined as

Figure 1. A typical alignment of the magnetic field devices
for BL23. The beam goes through from left to right.

55

Research and Development Highlights

MLF Annual Report 2014

4. Results of the calculations of polarization
We estimate the change of polarization along thebeam route to optimize the alignment of the magnetic
devices in a way which minimizes the depolarization.
Figure 2 shows typical results of the calculated polarization based on the found optimized alignment. The position of each device is indicated with arrows in Fig. 2(a).
The calculations were done on the line at the beam center (Y = 0 cm: Fig. 2(b)), and at the 3 cm above (Y = +3 cm:
Fig. 2(a)) and below (Y = −3 cm: Fig. 2(c)) the beam center. The red and blue lines indicate the angle, θB, between the spin and the magnetic field and the neutron
polarization, Pn, respectively. For this calculation, theneutron energy was 60 meV. θB becomes slightly worseat z~15 cm because the direction of the magnetic fieldchanges from horizontal to vertical in the area between
the solenoid coil and the vertical guide magnet (z =0.15~0.25 m). However, this does not affect significantly
the polarization. Pn is almost constant at Y = 0 cm and+3 cm along the beam route. The polarizations at theentrance of the analyzer housing are indicated at theright-top of the figures. Even for Y = −3 cm (Fig. 2(c)),

Pn = 0.96 is obtained. These values are satisfactory forpractical polarization experiments. Moreover, we havefound a criterion from the calculations that depolarization can be avoided if the amplitude of the magnetic
field is larger than 20 G. We also confirmed the alignment ensures satisfactory polarization in the energy region between 5 meV and 100 meV, which is the target
region of BL23. The results mean that we can construct
the magnetic field circumstance in BL23, which gives
minimized depolarization for white neutrons using theobtained alignment.
5. Measurements of magnetic field distribution
To confirm the reliability of the calculations of themagnetic field distributions in Sec.4, we measured magnetic fields using a real size test-bench of the magnetic
devices whose alignment is the same as the optimized
one in Sec.4. Figure 3 shows a picture of the test-bench,
which consists of guide magnets, and a Helmholtz
coil. The test bench does not include the supermirror
housing. The magnetic fields were measured with a 3D
gaussmeter.

Figure 2. Position dependence of neutron polarization (blue: right axis) and the angle, qB, between neutron spin and magnetic field(red: left axis) obtained by the calculations. The neutron energy is 60 meV. (a), (b) and (c) are the results at the beam center,the line at 3 cm below and above the center, respectively.

56

MLF Annual Report 2014

Research and Development Highlights

Figure 3. A picture of the test bench for magnetic field measurements.

Figure 4 shows an amplitude of the magnetic field
perpendicular to the beam route obtained by the calculation with ANSYS (red line) and by measurements
using the test-bench. The Helmhortz coil generated avertical magnetic field at the sample position. For themeasurements, the solenoid coil and the 3 cm guidecoil in Fig. 1 were not used. The observed magnetic
fields after the Helmholtz coil is lower than the calculations because the test-bench does not include the analyzer housing, which generates a strong magnetic field.
Excluding this region, roughly speaking, the agreement
is satisfactory. Note that the observed magnetic fields
between the Helmholtz coil and the fan shaped-verticalmagnet (z~80 cm) is about 20 G, which is not smaller
than the criterion value (~20 G) shown in Sec.4. Since
the effect of the analyzer housing increases the amplitude of the magnetic field as shown in Fig. 4, the depolarization around z~80 cm can be decreased. Though
the observed magnetic field between vertical guidemagnet and the Helmholtz coil (z~15 cm) is not consistent with the calculation, the observed magnetic fieldat the minimum point at z~10 cm is about 35 G, whichis larger than the criterion value (~20 G). Based on theseresults, it is expected that the optimized device alignment obtained in the calculations in Sec.4 could provide satisfactory polarization in BL23 of up to 100 meV.
This work is partly supported by the S-type projectof KEK (2009S09, 2014S09). The calculations were performed under the inter-university cooperative research

Figure 4. Amplitude of the magnetic fields perpendicular tothe beam obtained by calculations (red lines) andobservations (blue points). The origin of the horizontal axis is the right edge of the square-shapedvertical guide magnet. The upper and lower panels
are results of the magnetic field distribution at thebeam center and that along the line at 3 cm below
the beam center.

program of the Center for Computational Materials
Science, Institute for Materials Research, Tohoku
University (Proposal No.: 13S0416, 14S0413)
References[1] K. Ohoyama, T. Yokoo, S. Itoh, J. Suzuki, K. Iwasa, T.J.
Sato, H. Kira, Y. Sakaguchi, T. Ino, T. Oku, K. Tomiyasu,
M. Matsuura, H. Hiraka, M.Fujita, H. Kimura, T. Sato, J.
Suzuki, H.M. Shimizu, T. Arima, M. Takeda, K. Kaneko,
M. Hino, S. Muto, H. Nojiri, C.H. Lee, J.G. Park, and S.
Choi, J. Phys. Soc. Jpn. 82 (2013) SA035.
[2] T. Yokoo, K. Ohoyama, S. Itoh, J. Suzuki, K. Iwasa, T.
J. Sato, H. Kimura, N. Kaneko, and M. Ohkawara, J.
Phys.: Conf. Ser. 502 (2014) 012046.

K. Ohoyama1, T. Yokoo2,3, S. Itoh2,3, M. Sakaguchi2,3, M. Ohkawara4, Y. Nambu4, T. Ino2,3, and N. Kaneko2,3
Ibaraki University; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center; 3Institute of Materials Structure Science,
KEK; 4Institute for Materials Research, Tohoku University

1

57

Neutron SourceNeutron Source

MLF Annual Report 2014

Progress of the Neutron Source Section
1. 3-GeV proton beam transport facility
In fiscal year 2014, the 3-GeV Proton Beam Transport
Facility (3NBT) steadily delivered proton beam witha power of 300 kW extracted from the 3-GeV Rapid
Cycling Synchrotron (RCS) to the neutron production
mercury target until the summer shutdown period.
After the mercury target vessel was replaced in thesummer shutdown period, the 3NBT delivered a 300kW beam to the new mercury target until March, 2015,
and a 400-kW proton beam since then.
On January 12, 2015, for the first time proton beampulses were accelerated to a power equivalent of 1 MWin the 3-GeV RCS and successfully delivered to the neutron production mercury target through the 3NBT facility. It was a memorable moment for the Materials andLife Science Experimental Facility as an important milestone towards steady operation with a 1-MW beam.
Furthermore, we made efforts to reduce the beamloss through the beam transport line, especially fromthe muon target to the neutron production target. For
example, a beam tuning tool was developed with theStrategic Accelerator Design (SAD) system to optimize
the operational parameters of the magnets so that thebeam loss could be minimized. An automatic beam orbit adjustment system was developed to compensate
for the change of the magnetic field on the primarybeam line at the muon target when the solenoid magnet of the ultra-slow muon beam line is turned on.
2. Mercury target system
The neutron production mercury target has been
operated steadily at a beam power of 300 kW with mitigating pressure waves induced in it successfully thanks
to the gas micro-bubbles injection. The accumulated
beam power on the target reached 2050 MWh at theend of June, 2015.
The mercury vessel was replaced with an advanced
type. As shown in Fig. 1, the new target vessel has adouble-wall structure with a narrow mercury flow
channel with 2 mm width at the target front. Part ofthe mercury flow is led into the narrow channel witha flow velocity of 4 m/s without passing through the
bubbler, a gas micro-bubbles generator. The rest of theflow passes through the bubbler and advances to theinner wall with micro-bubbles. This structure enhances
the cooling performance of the inner wall, making it
possible to increase the wall thickness from 3 to 5 mm.
This prolongs the life time of the target front preventing
60

cavitation damage from operations with higher beam
power.

Figure 1. Illustration of cross sectional plane view of the mercury target vessel with double-walled target front.

We cut out a disk-shaped specimen from the target vessel front with a remote-handling cutting device.
Unfortunately, the specimen fell inside the target vessel, as shown in Fig. 2. However, we could observe themercury flow facing surface of the specimen, and did
not observe damages there. This was a proof of thepressure wave mitigation with the gas micro-bubbles
injection. Based on this promising result, we upgraded
the operational proton beam power from 300 kW to
400 kW in March, 2015.

Figure 2. Photograph of the disk-shaped specimen in the target vessel. The dotted line indicates the outline of
the specimen.

3. Effort to suppress tritium release during the mercury target vessel replacement operation
During the first target vessel replacement operation in 2011, a certain amount of tritium was released
when surrounding air penetrated the target vessel
while operations such as specimen cut-out from thetarget front and target vessel removal from the target
trolley were performed. Major mechanism of the tritium release is the isotope exchange reaction between

MLF Annual Report 2014

the air moisture and tritium stuck in the target vessel.
The accumulated beam power on the first target was
450 MWh. Considering that it was 2050 MWh on thecurrent target vessel and the allowable radioactivity at
the stack, it was needed to reduce the tritium release as
much as possible.
To meet the requirement, we introduced a process
to evacuate the target system by an off-gas processing system when surrounding air penetrated the target vessel (see Fig. 3). We also put plugs in the mercury
pipes of the target vessel after it was removed fromthe target trolley. As a result, the amount of tritium released through the stack was suppressed remarkably
to as low as about 12.5 GBq. This was only about 5.4%of the estimated value. It was a promising progress for
us because the target is planned to be irradiated toreach an accumulated power of 5000 MWh or more in
the future.

Neutron Source

4. Progress of the spare components fabrication2014 was the second year of a 6-year project toprepare moderators and a reflector. We continued thefabrication of a coupled moderator and a reflector. We
employed new material of Au-In-Cd alloy with a composition of 74.9 : 0.5 : 24.6 in at% for the de-coupler to
get neutron pulse with narrow shape. We made the AuIn-Cd alloy with a crucible and processed it to a plate
configuration. And then we contacted it with aluminumalloy, the structural material of the reflector, by meansof the Hot Isostatic Pressing method. It is estimated thatthe residual radioactivity of the used moderator and reflector assembly could be reduced to one-thousandthof that induced in the current assembly in which the
Ag-In-Cd alloy was installed as the de-coupler.
We also started the fabrication of a new de-coupledmoderator in which the Au-In-Cd alloy is used. Call forbids on the poisoned moderator was opened in the endof 2014.

Figure 3. Conceptual drawing of the off-gas process system and the mercury target system.

H. Takada
Neutron Source Section, Materials and Life Science Division, J-PARC Center61

Neutron Source

MLF Annual Report 2014

Status of Proton Beam Commissioning at MLF
1. Beam commissioning status
In Japanese Fiscal Year (JFY) 2014, a beam for neutron and muon production with power of 300 kW had
been steadily delivered. During the summer shutdown
period, the LINAC’s front end such as the ion source and
RFQ was replaced to accelerate a beam with peak current of 50 mA to achieve the designed beam power of
1 MW. After the replacement at the LINAC, some shotsof the beam were extracted from the 3-GeV rapid cycling synchrotron (RCS) to the beam dump and successfully delivered to the mercury target placed at the MLF
during the beam study. In the end of JFY2014, a steadybeam delivery has started with power of 400 kW.
As topics of the beam commissioning, two subjects
are described below: 1) Examination of the purificationof the cooling water for the muon production target
and magnets placed at the M2. 2) To mitigate the damage at the mercury target vessel, beam flattening system based on octupole magnets was used to reduce
the peak current density at the target.
2. Examination of cooling water purification
To isolate electrically the magnet coils from theearth, ceramic insulators were placed at the inlet andthe outlet of the cooling channel. At the magnet, copper was employed as a hollow conductor of the coil.
Last year, it was found that copper adheres to the insidewall of the magnet insulator at the upstream section,
which may lead the short circuit of the coil. To avoid theadherence, we concluded that the water should be frequently replaced. For the cooling of the muon production target and the magnets in the vicinities, a coolingwater loop, called 20 system, was installed at the MLF.
Although the system is dedicated to serve the muonsource, 3NBT is responsible for it for historical reason.
Due to the interaction at the muon target, 8% of thebeam is lost. As a result of the radiation caused by thebeam loss, the cooling water is high activated, which
was thought to be proportional to the beam power.
About 5% of the total water flow introduced into theion exchange resin to decrease the impurities caused byerosion at the cooling channel of the magnet has highactivation. After the beam operation, high dense tritium
and Be-7 was observed in the water by the measurement performed by radiation safety group with liquid
scintillator and gamma spectrometer. The tritium production rate normalized by the integration of the beam
power was constantly observed as 0.2 Bq/cm3/MWh,62

which showed good agreement with the result fromthe PHITS code. On the contrary, the production rateof Be-7 was scattered from 1 × 10−4 to 0.1 Bq/cm3/MWh.
Even though the density of Be-7 at the discharge line
for the 20 system was much lower than the value prescribed by the Japanese law, the local government required us to decrease the radiation to an undetectablelevel at the transfer line discharging the water into theocean so that decrease of the Be is required.
To match this condition, we decided to install an
additional purification system employed with the ion
exchange resin. To estimate the capture rate of Be at
the ion resin, the Be-7 density was measured by using
actual waste water and test loop. In the examination,
Be-7 density was measured at the initial condition. After
1 h flow of the loop, the density was measured again. It
was found that the ion exchanger resign reduced 99.9%
of Be-7, which indicated 1/1000 of the density. In JFY
2014, the system will be fabricated and will be installed
during the summer of 2015.

Figure 1. Status of magnet insulator adherences of copper at
inside.

3. Development of beam flattening system
Since pitting damaged at the mercury target vessel
is known to be proportional to the 4th power of peakintensity of the proton beam, it is required to decrease
the peak intensity so a beam flattening system wasdeveloped for that purpose. The 3-GeV proton beam
extracted from the RCS is well described by a simple
Gaussian. With ordinary beam optics, the beam shaperemains a Gaussian at all positions. Using nonlinear
optics with octupole magnets, the beam particles located at the beam periphery are deflected toward thebeam center, which flattens the beam distribution. To
obtain a flat distribution in both the horizontal andMLF Annual Report 2014

vertical directions, two octupole magnets are required.
In FY2013, octupole magnets were installed at the beamline shown in Fig. 2. After replacement of the muon production target from fixed type to rotating one, octupole
magnets can be fully utilized for user beam operation.

Neutron Source

octupole magnet must be 250 π mm mrad and β is set
to 200 m at the octupole magnets.
In January, 2015, the beam profile was measured bya profile monitor placed at 1.8 m upstream of the mercury target for the case of with and without octupole
magnets. The obtained beam profile is shown in Fig. 3.
Although some disagreement existed between experiment and calculation, the beam shapes were found to
be controlled as predicted in the design calculation. By
excitation of the octupole magnet, the beam halo wasconverged to the target center. It was also found thatthe heat and the dose of neutron produced at the target vicinity such as shielding and reflectors decrease.
The calculations indicate that, by introducing octupole
magnets, the peak current density can be reduced by
30%. Note that the present nonlinear optics systemrepresents the first attempt to install such a system in a
MW-class hadron accelerator.

Figure 2. Octupole magnet installed at the beam transport.

In order to obtain a flat beam distribution withan octupole magnet, the beam width at the octupole
magnet is expanded to a large β amplitude, which
is proportional to the square root of the beam width.
The physical aperture of the quadrupole magnets was
fixed at 300 mm; therefore, we set the physical apertureof the octupole magnets to 300 mm. For linear beam
optics, the admittance of the beam is designed to be
324 π mm mrad, which is given by the beam collimatorplaced at the RCS. A recent study of the RCS shows thatthe transverse emittance will be reduced to as little as
250 π mm mrad. Therefore, the beam admittance at the

Figure 3. Beam profile in horizontal direction obtained bybeam monitor placed at the entrance of the neutron target compared with calculation with (cyan)
and without octupole magnets (black) and muon
production target (red).

S. Meigo1, M. Ooi1, A. Akutsu1, T. Kawasaki1, M. Nishikawa1, and H. Fujimori2
Neutron Source Section J-PARC Center, JAEA; 2Muon Section J-PARC Center, KEK

163

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MLF Annual Report 2014

Operation Experience for Mercury Target in 2014
1. Introduction
In the summer of 2014, the mercury target vessel
was exchanged to #5 from #3. The target #3 had been
operated since January, 2012, and the injection of gasmicrobubbles into mercury was started in October,2013. The injection of helium gas microbubbles into
mercury is one of the prospective technologies available to reduce pressure wave induced cavitation.
In the process of proton beam injection into themercury target vessel, pressure waves are generated in
mercury by rapid heat deposition due to proton beamincidence. Negative pressure waves were generated
near the target vessel during the pressure wave propagation due to the difference in the sound impedance
between mercury and the target vessel. This negative
pressure generates cavitation, which causes severe
erosion damage to the target vessel. This damage determines the service life of the target vessel. If gas microbubbles are injected into mercury, microbubbles
absorb and attenuate the pressure waves and mitigate
the damage due to cavitation erosion. A gas microbubble generator had been developed and installed in the
mercury target vessel #3 [1].
Before exchanging the target vessel, the beam window portion of target vessel #3, where the severe damage was predicted, was sampled by using an annularcutter to evaluate the effect of the gas microbubble
injection on cavitation damage formation, and to produce specimen for post-irradiation examination.
The operation of the newly installed target vessel#5 started in November with beam power of 300 kW. In
March, 2015, the beam power was increased to 400 kW. Immediately after the operation with the new target
vessel started, a wrong alarm from the mercury detector was raised.
2. Cutout and inspection of the target vessel
The cutting was performed in a hot-cell using a
remotely controlled cutting machine with an annularcutter with outer diameter of 55 mm. The cutting was
performed without any coolant. In the process, the innermost specimen fell inside the vessel. The fallen specimen was not retrieved from the target vessel becauseof concerns regarding the contamination control inside
the hot-cell.
Video inspection with a CMOS camera was performed to observe the cavitation damage inside theinterior surface of the beam window region. Since the64

equivalent dose rate of the beam window was approximately 320 Sv/h, signal noise was superimposed on theimages obtained using the CMOS camera. The inspection did not obtain a clear image of the interior surface
demonstrating cavitation damage mitigation by thegas microbubble injection. Two of the three cameras
used herein were damaged during the inspection because of high doses of radiation.
Figure 1 shows the photographs of the inner surface of the beam window of target vessel #3 and across section of the cut hole obtained by the radiation
proof camera. It can be seen that the large machining
swarf that suggest the remaining of ductility on specimen. Furthermore, no obvious cavitation damage wasnoticed. In the cross section of the cut hole, the severe
cavitation erosion and V-shape erosion that was observed at the SNS target vessel was not registered here.
The conclusion is that the cavitation damage due to theproton beam-induced pressure waves was dramaticallyreduced by the gas microbubbles. Although it was impossible to quantitatively measure the damage depth,
it seems that the depth was less than 0.25 mm of thedepth obtained from target vessel #1, because it wasobserved that the concave surface of the inner wall was
relatively smooth.

Figure 1. Captured images of the cut specimen and cut surface of target vessel #3.

3. Wrong alarm from the mercury detector andcountermeasures
Immediately after the operation with target vessel #5, an alarm indicating that mercury leaked into
the safety shroud surrounding the mercury vessel was
raised. The leakage of mercury into the safety shroud
was detected by the electric resistance between thetarget vessel and the wire set in the shroud. To reset thealarm, the mercury should be removed from the space
between the vessel and the wire. However, the alarm

MLF Annual Report 2014150

Voltage (V)

100
50
0
-50
-100
-150
0

0.02

0.04
Time (s)

0.06

0.08

Figure 2. Time history of the voltage between the target vessel and the mercury detector when the false alarm
was raised.

Neutron Source

could be reset without removing it. We assumed that it
was a false alarm and started an investigation. Figure 2
shows the history of the electrical voltage between
the target vessel and the wire. Alternative voltage of
50 Hz was applied between the target vessel and thewire. Noises were observed every 40 ms (25 Hz), whichhave the same frequency as the beam injection. Hencenoise-cut filter was installed between the target vessel
and the wire. It was effective in killing the noise and thefalse alarm.
Reference[1] H. Kogawa et al., J. Nucl. Sci. Technol. 52 (2015)1461.

H. Kogawa, T. Naoe, T. Wakui, and K. Haga
Neutron Source Section, Materials and Life Science Division, J-PARC Center65

Neutron Source

MLF Annual Report 2014

Development Status of the AuIC Decoupler
1. Introduction
Thermal neutron absorber, called “Decoupler” is used
for producing neutron beams with sharp pulse shape. The
new gold-indium-cadmium (AuIC) alloy as a decoupler
is expected to have a better capability of reducing theresidual radio-activity than the previous silver-indiumcadmium (AIC) one [1]. This AuIC will be installed to sparemoderator-reflector assembly. In order to implement
Au-In-Cd alloy as a decoupler, it is to be bonded with analuminum alloy (A5083), which is a part of the structural
material of moderator and reflector, to remove the highheat deposition by neutrons from the mercury target
during high intensity proton operation. By adopting the
hot isostatic pressing (HIP) method, an optimal HIPing
condition was also found for a small size case with dimensions of 30 mm in diameter and 2 mm in height to assurea required bonding strength of more than 30 MPa [2].
However, there was still a critical engineering issue of theactual fabrication of moderator-reflector assembly withenlarged size. We report on the development status of
AuIC decoupler, especially for reflector assembly.
2. Development status of AuIC decoupler for reflector assembly
In order to install AuIC alloy to the neutron beamhole of the actual reflector assembly, we produced the
AuIC plates with dimensions of 2 or 3 × 130 × 130 mm
from AuIC alloy ingots. These plates were cut to proper
shape by using wire cutting (WEDM) to spread along
the neutron beam hole and cover it. The thickness of
the AuIC alloy plate was satisfactory within ±10% of
the thickness requirements, however, it was noticeable
that the plate had lumpy surface. HIPing without surface treatment would not provide the necessary bonding strength, which was observed in the previous study
between AIC and aluminum alloys. We performed small
sized HIPing tests with three different surface treatment
conditions, such as no surface treatment, emery paper
grinding up to 500 grift, and up to 1200 grift, to investigate the effect of bonding on the HIPing process. HIPing
was performed under the condition of 535°C, 100 MPa
and 1 hour holding time, which is optimal HIPing conditions for a small size case. Regardless of the surface treatment, the tensile strength gave over 90 MPa, which was
3 times higher than the required one. In the tensile test,
M. Ooi, M. Teshigawara, M. harada, and G. Noguchi
Neutron Source Section, Materials and Life Science Division66

fracture position was bonding area. The surface treatment with emery paper grinding up to 500 grift was applied for actual sized HIPing. Before actual sized HIPing,
middle sized HIPing (100 × 100 mm) test was performed
to confirm the effect of the enlarged size, such as thetensile strength and the bonding area. HIPing was performed under the same HIPing conditions, small sized,
as mentioned above. Separation at the bonding area
was not observed. Result of the tensile test also gaveover 80 MPa, and the fractured position was bonding
zone. We performed an actual sized HIPing of the reflector assembly based on the obtained results. After HIPing,
the HIPed block was machined to parts of the reflector,
which had neutron beam holes. AuIC plates were embedded in the neutron beam holes. No separation was
found at the embedded area after ultrasonic inspection,
as shown in Fig. 1. At present, we are continuing to thenext step, fabricating a spare reflector.

A5083
3

A
AuIC
Figure 1. Ultrasonic inspection of the neutron beam hole of
the reflector. The AuIC plates are embedded in theneutron beam holes. No separation was found by
ultrasonic inspection.

Acknowledgment
We thank for the cooperation of Metal Technology
Co. Ltd. to fabricate the spare reflector assembly. We
also thank the NAT staff for their help.
References[1] M. Harada et al., Journal of Nucl. Mat. Vol. 398 (2010)
pp.93-99.
[2] M. Ooi et al., Journal of Nucl. Mat. Vol. 450 issue 1-3(2014) pp.117-122.

MLF Annual Report 2014

Neutron Source

Upgrade of the MLF Control Network System
1. Introduction
At the Materials and Life Science Experimental
Facility (MLF), four LANs are supported. One of them,
J-LAN, serves for the MLF users. The rest, which are used
for facility control, are called 3NBT-Control-LAN, MLFControl-LAN and MLF-Monitor-LAN. The 3NBT-ControlLAN is used for control of the 3 GeV proton beamtransport line (3NBT), is located in the 3NBT building and the north side of the MLF building. The MLFMonitor-LAN monitors MLF’s network cameras, whose
number exceeds 100. The network traffic of the cameras is normally high and that traffic is isolated from the
MLF-Control-LAN. The MLF-Control-LAN is used for the
MLF control system which controls many instruments
for both the neutron source facility and the muonsource facility in MLF.
2. Objective
The network hardware of the 3NBT and MLF was
designed as a part of the J-PARC control LAN which
was installed from 2005 to 2007. This network system
is maintained and extended, but eventually it ages andneeds gradual replacement. So, we have performed
replacement and upgrade of the network system, including network speed enhancement. In the MLF, thesystem’s replacement has been planned for the period
between 2013 and 2015. Although it takes three years,
the operation of the MLF must continue during thistime. High reliability would be required even if old andnew network systems are mixed.
3. Equipment
The concept of the redundant network system of
J-PARC is shown in Fig. 1. Taking into account the factthat the future traffic load and network speed between
the MLF and CCR would increase, we upgraded the 1st
and 2nd edge switches of 20 Gbps network speed for the
MLF and 10 Gbps for the 3NBT, and the terminal switches of 1000 MBps. In addition, the 2nd edge switches andthe important terminal switches are duplicated basedon the concept of the redundant system. Models of
the previous and the new LAN switches are shown in
Table 1.

Figure 1. Concept of the redundant network system of J-PARC.

Table 1. list of the LAN switches.
Previous

Replaced

1st Edge switch

BlackDiamond
BD6804

Summit X650

2nd Edge switch

Alpine 3804
Summit48si

Summit X480

Terminal switch

Allied Telesis switch

Summit X440

4. Summary
The LAN switches have been replaced graduallyfrom 2013 to 2015 in the following regions:2013: 3NBT and 1st Edge switches of the MLF
2014: MLF Control-LAN
2015: MLF Monitor-LAN.
As the maintenance period in J-PARC is scheduledfrom July to September, our upgrade, including thesystem check after replacement, had been done in thisperiod of every year. The replacement works will becompleted by September, 2015.
Acknowledgement
We thank to Kikuzawa, Kawase and Yukawa for their
help with this work.

M. Ooi, K. Sakai, and A. Watanabe
Neutron Source Section, Materials and Life Science Division

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MLF Annual Report 2014

Neutron Science Section
1. User Program
In the 2014A and 2014B proposal rounds, 17
neutron instruments were in operation for users and603 proposals were applied to them. The number increased dramatically from 475 in 2013. 345 proposals or
57% of the proposal applications, were approved. The
reserved ones were 81 and the rest were not approved.
The beam operation scheduled from January 17 washighly affected by the fire accident in the muon area in
MLF and the problems at RCS and the neutron source,
so a total of 33.5 days of user beamtime was lost. The
experiments, which could not be carried out in the termfrom January to March, were carried over into 2015 as
exceptional measures.
2. Instruments development and construction
The layout of the neutron instruments at MLF as ofthe end of JFY 2014 is shown in Fig. 1.

22, 2014 (Fig. 2). Since then, the VIN ROSE has been
under commissioning. The performance of the beamtransport system has been evaluated and the devices
tuned.

Figure 2. First beam of the VIN ROSE.

At BL22, the energy-resolved neutron imaging system, RADEN, was installed by JAEA as a public beamline instrument. The RADEN received the first neutron
beam on November 4, 2014. Test imaging measurements of several samples are in progress. An example
is shown in Fig. 3.

Figure 3. First imaging on RADEN.

Figure 1. Layout of the neutron instruments at MLF as of JFY
2014. BL06 & 22 had proceeded to the commissioning phase in this fiscal year. BL23 remained underconstruction.

Kyoto University and KEK installed the VIN ROSE
at BL06, which consists of a neutron resonance spinecho (NRSE) instrument and a modulated intensity by
zero effort (MIEZE) instrument. The construction of theshielding and the interlock system was completed andthe VIN ROSE received the first neutron beam on April
70

3. International Activities
MLF held the 2nd MLF School from December 16
to 19. 22 students (13 from Japan, 9 from foreign countries) participated and enjoyed lectures and actual experiments using muon and neutron beams (Fig. 4). The
Neutron Science Section contributed to the neutron
part of the school. 7 neutron instruments were provided for practical experiments.
The 14th Korea-Japan Meeting on Neutron Science
was held from January 7 to 9 at the Ibraki Quantum
Beam Research Center. 50 Japanese and 29 Korean

MLF Annual Report 2014

scientists participated and recent scientific and instrumental topics were presented in 59 oral and poster presentations. Also, the future plans for the Korea-Japan
collaboration in neutron science was discussed. (Fig. 5)

Figure 4. MLF school students performing thier experiment
at SIKI, BL01.

Figure 5. Participants of the 14th Korea-Japan Meeting on
Neutron Science.

4. Resultant outcomes
The research activities in neutron science at MLF
resulted in more than 110 papers. The number includes

Neutron Science

articles in influential journals such as Nature Physics,
Nature Communications.
Two staff members, Dr. H. Nakagawa and Dr. N. L.
Yamada won the Encouraging Prize of the JapaneseSociety for Neutron Science. Prof. M. Hino of Kyoto
University received the Technology Prize from theJapanese Society for Neutron Science for his work indeveloping neutron optical devices for VIN-ROSE.
We distributed 6 press releases on scientific outcomes and technical development from our beam lines:࣭ Combination of neutron and X-ray inelastic measurement reveals the whole scheme of electron
excitation states: Electron doping effect on highenergy magnetic excitations in high-Tc cuprate.
(Apr. 25, 2014)
࣭ How does water define the shape of DNA?: Local
dynamics coupled to hydration water determines
DNA-sequence-dependent deformability. (Aug. 29,
2014)࣭ Combination of neutron and X-ray inelastic measurement reveals the whole scheme of electron
excitation states: Electron doping effect on highenergy magnetic excitations in high-Tc cuprate.
(Apr. 25, 2014)
࣭ Finding hydrogen in Iron dissolved under highpressure: Determination of site occupancy of interstitial deuterium atoms in face-centred cubic iron.
(Sep. 26, 2014)
࣭ New elemental analysis realized with J-PARC:
Development of Time-of-flight prompt gamma-ray
analysis (TOF-PGA) for multi-elemental analysis.
(Dec. 22, 2014)
࣭ New hydride with Cr: Predicted by the first principle
calculation and confirmed by neutron scattering.
(Mar. 24, 2015)

K. Nakajima1, Y. Kawakita1, S. Itoh1,2, and T. Otomo1,2
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, High Energy
Accelerator Research Organization, KEK

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BL01: 4D-Space Access Neutron Spectrometer 4SEASONS
1. Introduction
4SEASONS is a thermal neutron Fermi-chopper
spectrometer for inelastic scattering measurements,and one of the Public Beamlines in MLF [1]. It is operated by 6 instrumental scientists and 1 dedicated engineer. In fiscal year 2014, 37 General Use proposals,
including 2 trial ones, were applied for, and 27 of themwere approved. 8 proposals were submitted by international users. The major research field was strongly
correlated electron system and magnetism, which
dominated 70% of the General Use proposals in 2014.
The high interest in these research fields seems to benatural considering that 4SEASONS was originally constructed for the research project of the copper oxide
high-temperature superconductivity [2]. However, it
should be noted that a sizeable number of proposals
belong to other research fields such as thermoelectricmaterials and catalysts. In addition to the General Use
proposals, one Strategic Use proposal for the ElementStrategy Project for electronic materials was submitted
and approved. Unfortunately, a few of the approved
proposals were postponed for 2015 because of an unexpected long-term shut-down of MLF.
2. Development in the Fermi chopper
The original Fermi chopper of 4SEASONS holds
a slit package with 65 × 70 mm cross-section and100 mm depth. Its designed maximum rotation frequency was 600 Hz [1]. However, in 2011, it was foundthat the rotation was unstable at high frequencies because of a secular change of the slit package, and werestricted the rotation frequency at 350 Hz and lower.
This situation restricted severely the available energy
resolutions, especially for high-energy experiments.
Accordingly, we developed a new Fermi chopper,
which was manufactured by MIRROTRON Ltd. and SKF
Magnetic Bearings (Fig. 1). The new Fermi chopper hasa more compact slit package whose cross-section anddepth are 58 × 53.4 mm and 20 mm, respectively. The
spacing of the slits is designed so that it gives the sameenergy resolution as the original chopper. Thanks to thecompact design, it can rotate stably at up to 600 Hz.
Another important benefit of the shallow depth slits isthat the chopper provides much higher neutron transmission than that of the original chopper particularly
for low energy neutrons and high rotation speeds [3].
A test measurement with the new chopper performedin the end of fiscal year 2014 showed that the ratio of72

Figure 1. The Fermi chopper translation unit with the original and new Fermi choppers being installed on
4SEASONS by the technical support staffs.

available neutron flux between the new chopper andthe original chopper is, for example, 1.9 for 43 meV neutrons and 250 Hz rotation. It reaches even 17 for 18 meVand 300 Hz. The new Fermi chopper will be available forthe users program in 2015.
Simultaneously, we are developing another Fermi
chopper, called MAGIC chopper, which utilizes supermirror-coated slits [4]. In 2014, we operated the prototype of the MAGIC chopper on BL01. Although theavailable neutron flux was much lower than the expected values due to the low reflectivity of the utilized
supermirrors, we verified successfully the basic performance of this type of chopper. Now we are developing
a new slit package with higher-reflectivity supermirrors.
3. Increase of detectors
The vacuum scattering chamber of 4SEASONS isequipped with 11 detector banks. Each of the detector banks can hold 32 pieces of 2.5 m-long 3He position
sensitive detectors, and the whole set of detector banks
can provide scattering angle in the range of −35.3° −+130.5° in the horizontal [1]. However, the detectorbanks are not fully occupied due to the recent shortage and the resulting higher price of 3He gas, and it isdesired to fill as much vacancies as possible. Following
2013, we installed 33 pieces of detectors in fiscal year
2014, which resulted in the maximum scattering angle
in the horizontal of 84°. In addition, we have alreadypurchased another 13 pieces of detectors. They will beavailable in fiscal year 2015.

MLF Annual Report 2014

4. Background originating from delayed neutrons
Suppressing background scattering is critical forhigh-quality inelastic neutron scattering experiments,
and the background problem has been continuously
investigated on 4SEASONS. Recently we found that acontinuous background that oscillates in synch withthe rotation of the Fermi chopper was observed even in

Figure 2. (a) A time spectrum acquired by 4SEASONS. The
dashed line shows the background dominated bydelayed neutrons. (b) Magnified view of the panel(a) in the time range between 25 000 μs and 40
000 μs. Dashed and dash-dotted lines show times
when the Fermi chopper opens and rotates by π/2,
respectively [5].

Neutron Science

the time region when neutrons should be suppressed(Fig. 2). The characteristics of the background strongly
suggest that high-energy delayed neutrons continuously emitted from the mercury target are its cause [5].
A similar oscillating background was observed bya chopper spectrometer at the ISIS facility of theRutherford Appleton Laboratory when the facility useduranium as the neutron target [6]. The observation on
4SEASONS demonstrated that the effect of the delayed
neutrons is carefully considered even in facilities that
do not use fissionable targets.
References[1] R. Kajimoto, M. Nakamura, Y. Inamura, F. Mizuno, K.
Nakajima, S. Ohira-Kawamura, T. Yokoo, T. Nakatani,
R. Maruyama, K. Soyama, K. Shibata, K. Suzuya, S.
Sato, K. Aizawa, M. Arai, S. Wakimoto, M. Ishikado,
S. Shamoto, M. Fujita, H. Hiraka, K. Ohoyama, K.
Yamada, and C. H. Lee, J. Phys. Soc. Jpn. 80, SB025(2011).
[2] M. Arai et al., Grant-in-Aid for Specially Promoted
Research from MEXT (17001001).
[3] M. Nakamura and R. Kajimoto, JPS Conf. Proc. 1,
014018 (2014).
[4] M. Nakamura, M. Arai, R. Kajimoto, T. Yokoo, K.
Nakajima, and Th. Krist, J. Neutron Res. 16, 87(2008).
[5] R. Kajimoto, M. Nakamura, Y. Inamura, K. Kamazawa,
K. Ikeuchi, K. Iida, M. Ishikado, K. Nakajima, M.
Harada, and M. Arai, JPS Conf. Proc. 8, 036001 (2015).
[6] M. Arai, A. D. Taylor, S. M. Bennington, Z. A. Bowden,
R. Osborn, M. Kohgi, K. Ohoyama, and T. Nakane,
Proc. the 11th Meeting on Inter. Collaboration ofAdvanced Neutron Sources (KEK Report 90-25,
1991), p. 644.

R. Kajimoto1, M. Nakamura1, Y. Inamura1, K. Kamazawa2, K. Ikeuchi2, K. Iida2, and M. Ishikado2
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division CROSS-Tokai

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MLF Annual Report 2014

Oscillating Radial Collimators for the Chopper
Spectrometers at MLF in J-PARC
1. Introduction
Inelastic neutron scattering (INS) measurement using chopper spectrometers has greatly contributed tothe development of materials science. A chopper spectrometer is still a flagship instrument in high-power
pulsed spallation neutron source facilities, such as theMaterials and Life Science Experimental Facility (MLF)
in the Japan Proton Accelerator Research Complex(J-PARC). Even though the MLF provides a high-intensity neutron beam, the countermeasure against thebackground is indispensable in the INS measurement
due to the weak signal during the inelastic process.
Recently, INS measurements under high temperature orhigh magnetic field have been frequently required [1].
Obviously, the sample environment apparatus causes
unwanted scattering and affect the data quality. In order to overcome these background problems in the INS
measurement under special sample environment, wedeveloped oscillating radial collimators specifically forthe chopper spectrometers at MLF in J-PARC. A radialcollimator has been conventionally used to suppress
the off-sample parasitic scattering without perturbing the sample scattering [2, 3]. The performances of
newly-developed radial collimators will be described inthis report.
2. Design and Operation of Radial Collimators
We have developed two types of oscillating radialcollimators in-house based on the result of preliminary
evaluation tests for many kinds of shielding blades [4].
One is made of Gd2O3 shielding blades and the other of
Cd shielding blades. The total thickness of a Gd2O3 bladeis 100 μm, that is 25 μm Gd2O3 + 50 μm Mylar + 25 μm
Gd2O3. On the other hand, a Cd blade attached to a radial collimator has a total thickness of 150 μm (25 μm
Cd-plating + 100 μm 5052 aluminum alloy + 25 μm Cdplating). We have adopted the metal substrate for a Cd
blade in order to improve the performance in relatively
high-energy region. There is no difference in mechanical design between these collimators. A radial collimator can be attached on the conventional 800 mm
flange based on the sample environment (SE) protocol
of MLF. Also, a 400-mm flange can be prepared to allow the standard SE apparatuses, such as a cryostat,
to be mounted. Our collimator has an inner radius r of
210 mm, an outer radius R of 400 mm, and an angular74

separation α of 2.5°. The shielding blades cover therange from −45° to +135° in horizontal direction. The
blade length is given by R−r, which is 190 mm, and theblade height is 482 mm. Using these parameters, thediameter of visible sample d is calculated by

d=α⋅

Rr
R−r

where d is identical to the ‘maximum impact parameter’
introduced in Ref. [2]. Substituting parameters r, R, andα, the value of d for our radial collimator is estimated tobe 19.3 mm.
The oscillation of a radial collimator is driven by astepping motor placed in vacuum, and a feedthroughelectrical connection is used at the vacuum boundary.
An aluminum plate is used to transfer the generated
heat from the motor to the flange. The lubrications of
the driving elements are done with commercial ultrahigh vacuum grease. Linear motion produced by a ballscrew coupled to the motor is converted to rotary motion by a crossed roller bearing. The oscillating speed
is set to 0.04°/s. as default and the oscillation range is±2.5°. Each shielding blade is tautened by using tension
springs.
To evaluate the performance of each radial collimator, we performed neutron scattering measurementwith and without a radial collimator on 4SEASONS installed at BL01 of MLF [5]. The sample for the evaluation measurement was vitreous silica (v-SiO2) rod with
8.5 mm diameter which is much less than 19.3 mm. The
sample was set into the top-loading cryostat conventionally used at 4SEASONS. The dynamical structure
factors were obtained at room temperature with andwithout a Gd2O3 radial collimator. The Q dependencesof the elastic structure factor are given in Fig. 1. The incident neutron energies were 37.0, 80.7, and 300.0 meVusing the Multi-Ei method [6]. The unwanted scatterings
from the cryostat are represented by arrows in Fig. 1.
It was found that the Gd2O3 radial collimator could effectively shield the unwanted scattering from the cryostat window and provide us the high-quality data. The
shielding property of Gd2O3 is getting worse in thehigh-energy region, the large incoherent scatteringfrom a Mylar substrate significantly affects the data, as
shown in Fig. 1(c). However, the Gd2O3 radial collimator
provides enough performance for the experiments at

MLF Annual Report 2014

Neutron Science

Figure 1. Q dependences of the elastic structure factor for v-SiO2 with and without a Gd2O3 radial collimator. The diameter of v-SiO2
is 8.5 mm. The sample is set into the cryostat and the measurements are performed at room temperature. Incident neutronenergy is (a) 37.0 meV, (b) 80.7 meV, and (c) 300 meV.

Figure 2. Same as in Fig. 1, but with and without a Cd radial collimator. Cross symbols show the reduced intensity for the data without a Cd radial collimator. The reduced factor is 0.78 for all incident energies.

the chopper spectrometer with curved guide systemsuch as AMATERAS installed at BL14 of MLF [7]. The
spectrometer with a curved-guide system can avoid
the delivery of high-energy neutrons to the sample position. In fact, the best performance of AMATERAS canbe achieved in the energy range from 1 to 20 meV, andsufficient performance can be realized up to 80 meV.
Next, we shall discuss the performance evaluation
tests of the Cd radial collimator. Figure 2 represents
the experimental results for Cd radial collimator, where
the experimental conditions are the same as for Gd2O3
given in Fig. 1. The Cd radial collimator provides better
quality data in the high-energy region as expected. The
cross symbols in Fig. 2 represent the intensity without a
Cd radial collimator reduced by the factor of 0.78. The
reduced factor provides the same value for all incident

energies. It was also confirmed that the reduced factor
in the inelastic region was equal to 0.78. The diameterof the v-SiO2 rod was much smaller than the maximum
impact parameter 19.3 mm, and the experimental results for Gd2O3 shown in Fig. 1 have surely demonstrated the negligible intensity loss. The thickness of therespective shielding blades is certainly different, butgeometrically it cannot make a significant differencein the intensity loss between the Gd2O3 radial collimator and the Cd one. Keeping tension when using metal
substrate should be more difficult than in the case withMylar substrate. It seems reasonable to suppose thatthe unexpected intensity loss in the Cd radial collimatoris caused by this difficulty. In other words, there is room
for improvement in the current Cd radial collimator.

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MLF Annual Report 2014

3. Summary
We have developed two types of oscillating radial collimators for the chopper spectrometer at MLF in
J-PARC based on the evaluation test of shielding materials
as a blade for the radial collimator. One is made of commercially available Gd2O3 sheets designed for low-energy chopper spectrometers, and the other of Cd-plated
aluminum sheets for relatively high-energy chopper
spectrometers. The Cd radial collimator provides better
performance in the high-energy region than the Gd2O3
radial collimator, but it has shown a loss with unexpected
intensity. We are planning to investigate the causes andimprove the performance of the Cd radial collimator.

References[1] M. B. Stone et al., Rev. Sci. Instrum. 85 (2014) 085101.
[2] J. R. D. Copley et al., Nuclear Inst. and Meth. Phys.
Res., A345 (1994) 313.
[3] A. F. Wright et al., Nuclear Inst. and Meth. Phys. Res.,
A180 (1981) 655.
[4] M. Nakamura et al., JPS Conf. Proc. 8 (2015) 036011.
[5] R. Kajimoto et al., J. Phys. Soc. Jpn. 80 (2011) SB025.
[6] M. Nakamura et al., J. Phys. Soc. Jpn. 78 (2009)
093002.
[7] K. Nakajima et al., J. Phys. Soc. Jpn. 80 (2011) SB028.

M. Nakamura1,2, Y. Kawakita1, W. Kambara1,2, K. Aoyama1, R. Kajimoto1, K. Nakajima1, S. Ohira-Kawamura1, K. Ikeuchi3, T. Kikuchi1,
Y. Inamura1,2, K. Iida3, K. Kamazawa3, and M. Ishikado3
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Technology Development Section, Materials and Life Science
Division, J-PARC Center; 3Neutron R&D Division CROSS-Tokai

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Neutron Science

BL02: Current Status of the Broadband micro-eV
Inelastic Neutron Spectrometer DNA
1. Introduction
The time-of-flight (TOF) near-backscattering spectrometer (n-BSS), DNA, was constructed and started
operating in 2012 at the Materials and Life Science
Experimental Facility (MLF) of the Japan Proton
Accelerator Research Complex (J-PARC). It is an indirect
geometry instrument with Si crystal analyzers and sees
the coupled moderator of the pulsed spallation neutron source in MLF, which has the most intense but also
the widest pulse among all three moderators in MLF.
With the aim of a high energy resolution even with highintensity, DNA is the first n-BSS installed with a highspeed pulse-shaping disc-chopper in the world. The
purpose of DNA is to research, in nanosecond timescaleor with micro-eV resolution, the dynamical behaviors of
atoms and spins in bio-molecules, functional-materials,
strongly-correlated electron systems and so on [1, 2].
The instrumental overview and the present specifications of DNA are shown in Table 1 and Figure 1.
Table 1. Instrumental specifications of DNA.
Items
Specification
Neutron source (NS)
Coupled Liquid H2 Moderator
L1 (source-sample)
42 [m]
L2 (sample-analyzer)~ 2.3 [m]L3 (analyzer-detector)~2.0 [m]Pulse-sharpening chopper (PS-chopper)
Max speed: 300 Hz at ~7.5 m from NS(Present Max speed: 225 Hz by 4 slits on one disc)
Crystal Analyzer
Crystal and reflection index Si(111)Si(311) in test
Bragg angle of analyzers~87.5 [deg.]
Energy resolution~2.4 [μeV]: Si(111) with 10 mm Slit @225 Hz~3.5 [μeV]: Si(111) with 30 mm Slit @225 Hz~14 [μeV]: Si(111) without PS-chopper~12[μeV]: Si(311) with 10 mm Slit @225 Hz
Momentum range
0.08 < Q < 1.85 [A−1]: Si(111)0.60 < Q < 3.80 [A−1]: Si(311) in plan
Scan energy range:
Si(111): −40 < E/μeV < 100: Single pulse scan around Ef−400 < E/μeV < 600: Multi pulse scan around Ef−500 < E/μeV <1500:
without PS-chopper in second frame
Si(311): −150 < E/μeV <300: Single pulse scan around Ef(Specifications as of the end of March. 2015)

Figure 1. DNA 3D view (a) and inside of the scattering vessel (b).

2. Construction works and installation status until
2014
Almost all spectrometer components were installed before February, 2012, except the high-speed
pulse-shaping disc chopper. At this time, the commissioning work have been carried out without the pulseshaping chopper. The pulse-shaping chopper, which isdesigned as a counter-rotating double-disc chopperwith a maximum rotational frequency of 300 Hz, wasset up at a position of 7.75 m away from the moderator
into the interstice of the super-mirror neutron guides
and commissioned at 225 Hz rotational frequency inearly April, 2013. After that, the measurement using
the pulse-shaping chopper became the main measurement mode.
By the end of September, 2013, the coverage of theSi(111) crystal analyzers was extended to a scatteringangle range from -18 degrees to +138 degrees in thehorizontal plane by adding some analyzer units. That in
the vertical direction is in the range from +21 degrees
to −14 degrees. Neutrons scattered by the sample aremeasured by position-sensitive 3He gas detectors arranged on the same circumference of the scattering
center shifted upwards and downwards, after being
energy-analyzed (back-scattered) by the upper and thelower parts of the Si crystal analyzer units, respectively.
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MLF Annual Report 2014

These arrangements of the analyzer units and the detectors enable us to angle-resolve scattered neutrons
not only in horizontal but also in vertical directions
two-dimensionally, and therefore, DNA has a potential to carry out experiments even for single crystalline
sample.

References[1] K. Shibata, N. Takahashi, Y. Kawakita, M. Matsuura, T.
Yamada, T. Tominaga, W. Kambara, M. Kobayashi, Y.
Inamura, T. Nakatani, K. Nakajima, and M. Arai, JPS
Conference Proceedings, 8, 036022 (2015).
[2] N. Takahashi et al., Journal of the Physical Society ofJapan, 80, SB007 (2011).

K. Shibata1, Y. Kawakita1, M. Matuura2, T. Tominaga2, T. Yamada2, K. Nakajima1, W. Kambara1, M. Kobayashi2, Y. Inamura1,
T. Nakatani1, and S. Kasai2
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division CROSS-Tokai

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Neutron Science

IBRAKI Biological Crystal Diffractometer iBIX
1. Introduction
Single crystal neutron diffraction is one of the powerful methods to obtain structure information including that of hydrogen atoms. The IBARAKI biologicalcrystal diffractometer called iBIX is a high-performancetime-of-flight single-crystal neutron diffractometer toelucidate the hydrogen, protonation and hydration
structures of organic compounds and biological macromolecules in various life processes.
2. Current status of iBIX
Since the end of 2008, iBIX has been available foruser experiments supported by Ibaraki University [1].
In FY 2012, we successfully upgraded the 14 existing
detectors and installed the 16 new detectors for thediffractometer of iBIX [2]. The total measurement efficiency of the present diffractometer was higher by one
order of magnitude than the previous one, coupledwith increased accelerator power. In the end of FY 2012,
the use of iBIX in user experiments for biological macromolecules started on a regular basis. In FY 2014, theaccelerator power of J-PARC was 300 kW. We can collecta full data set of biological macromolecules for neutron structure analysis with around 2.0 Å resolution in
10 days by using iBIX. The size of the samples measured
by iBIX is from 1 to 6 mm3 in volume. If the accelerator power is increased to 1 MW, the total measurement
time or the sample size will be reduced to onethird of
the time needed before. In the beginning of FY 2014,
we collected successfully the diffraction data sets of
6 biological macromolecules over a period of about
4 months. Some interesting results were obtained fromthese experiments which shows the benefits from theneutron diffraction experiment.
3. Developments
We started the process of improving the data reduction method and upgrading the diffractometer instruments in order to increase the data accuracy for the
integrated intensities of Bragg reflections and make thesystem more user-friendly in the next phase of development of the instruments.
In order to carry out precisely the integration of
Bragg intensities, we should be able to predict precisely
the X, Y, TOF positions of Bragg reflections in the histogram data. In other words, the UB matrix should bedetermined precisely with the instrument parameters,such as detector positions and distance between themoderator and sample position L1 and offset angle ofgoniometer. Therefore, we determined the instrument
parameters by measurement of Bragg reflections of astandard sample. The L1. detector parameters of 30 detectors and goniometer offset angle were obtained andthen the accuracy of the indexing of Bragg reflections
and the refinement of UB matrix could be successfully
improved.
In order to improve the quality of the integrated intensity of weak reflections, we are aiming to implement
the software component of profile fitting to data reduction software STARGazer. We are trying to seek functions representing asymmetry intensity distribution
from the existing profile functions by using TOF powder
diffraction method and verify the usefulness of thesefunctions by the non-linear least square method. We
discovered successfully the most suitable profile function, which is back-to-back exponentials convolved
with a Gaussian. We will apply this function to profile
fitting in order to obtain accurately the integrated intensity of the weak reflections.
To respond to users’ various needs, we are developing new equipment of the sample environments.
Figure 1 shows the heating system for the fiber sample.
The attainable temperature is from room temperature
to about 300°C. Figure 2 shows the tension applying
device for the fiber sample. The specifications are as follows: stretching rate: 1~100 μm/sec, range of stretching: 90 mm, maximam load: 200 N. These parts of theequipment can be mounted on the multi-purpose
stage, which was developed in FY 2013. In FY 2015, we
will try to test measurement of sample environmentswith this equipment.

Figure 1. Heating system for the fiber sample.

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MLF Annual Report 2014

measured by iBIX, some neighboring Bragg spots will
overlap partially each other because iBIX was installedon the coupled moderator with a wide pulse shape. It
is necessary to de-convolute the overlapped spots inorder to obtain their integrated intensity, we will startthe development of the de-convolution component foroverlapped Bragg spots to obtain the intensity of eachone of them.
As of the hardware, we should carry out the commissioning of the utility equipment for sample environment that was developed in FY 2014 (e.g. heating andextension devices).
Figure 2. Tension applying device for the fiber sample.

4. Feature prospects
In FY 2015, we will continue the development of thedata reduction software to make it more user-friendly
and complete the work on the integration component
with the profile fitting method for weak reflection. In thecase of the diffraction data from larger unit cell crystals

References[1] I. Tanaka, K. Kusaka, T. Hosoya, N. Niimura, T. Ohhara,
K. Kurihara, T. Yamada, Y. Ohnishi, K. Tomoyori and T.
Yokoyama, Acta Cryst. D66 (2010) 1194-1197.
[2] K. Kusaka, T. Hosoya, T. Yamada, K. Tomoyori, T.
Ohhara, M. Katagiri, K. Kurihara, I. Tanaka and N.
Niimura J. Synchrotron Rad. 20 (2013) 994-998.

K. Kusaka1, T. Yamada1, N. Yano1, T. Hosoya1, I. Tanaka1, T. Ohhara2, and M. Katagiri1
Frontier Research Center for Applied Atomic Sciences, Ibaraki University, Tokai; 2J-PARC Center, JAEA

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BL04: Developments of New Data Acquisition System andTotal Cross-section Measurement Detectors at ANNRI
1. Introduction
A new data acquisition system (DAQ system) and a
new total neutron cross-section measurement system
are now being developed at the BL04 ANNRI facility(ANNRI) as a part of a research project entitled “Researchand development for Accuracy Improvement of neutron
nuclear data on Minor ACtinides (AIMAC)”. In ANNRI, twodifferent types of γ-ray detector systems are operated inorder to measure neutron capturing cross-sections. One
is a Ge detector system (Ge system), which has very fineγ-ray energy resolution, the other is an NaI detector system (NaI system) with wide neutron energy range measurement capability. Depending on the experimental
purpose, only one system is selected in each experiment.
Now, in ANNRI, an Li-glass neutron detector system(Li-glass system) is being developed for total neutron
cross-section measurement. In the case of a total neutron
cross-section measurement, the setup of detectors can include a neutron capture cross-section measurement without any experimental conflict. Once the development of
the total cross-section measurement system is completed,
ANNRI will be able to measure the total and capture crosssections simultaneously. In order to complete the projectsuccessfully, not only the Li-glass system but also the DAQ
system itself must be developed because the current DAQ
system cannot be applied to the Li-glass detector signal
as-is. Moreover, it will be difficult to maintain the current
DAQ for the Ge system due to its aging.
2. New DAQ system constitution
In order to measure the total cross-sections, boththe upstream and downstream sides of the measuring
sample must be collimated well to reduce the small angle scattering effects. In ANNRI, two collimator systems
are prepared. One is the rotary collimator on the upstream side of the Ge system, the other is the intermediate collimator between the Ge and NaI systems. As there
is no remaining space to set additional collimator on
the downstream side of the NaI system, the measured
sample must be located between the rotary collimatorand the intermediate collimator in the case of a total
cross-section measurement. As the Li-glass system must
be located at more than 1 m downstream from the NaI
system because of experimental limitations, simultaneous measuring mode is required to obtain detector data
at two separate positions at the same time. In order toovercome this problem, a new DAQ system is being designed by the TCP/IP protocol based client-server model.
The role of the client-side application is to gather
data from each ADC and send it to the server-side. The
server-side receives data from each client, builds one
event data block, and saves it to a disk. Each client is controlled by a common signal issued from the server-side
application. Basically, client and server applications aredesigned to be operated on different PCs, but if the IP address of the server application is set as localhost, this DAQ
system can be operated with only one standalone PC.
Inside the client-side application, the DAQ systembackend makes a parallel routine for each ADC board automatically. Without any modifications in the user sidecode, this DAQ system runs with linear scalability to the
ADC board number, up to the CPU core number minus
one. (One core is used for the DAQ system except for thecase of single core PC). The max data building rate is limited by the TCP/IP network speed limit. In local tests, thelocal area network speed in ANNRI was about 250 MB/s.
To digitize the detector signals, two different typesof ADCs are used. CAEN v1724 [1] 14-bit 100-MHz peakhold ADC boards are characterized by fine pulse height
digitizing resolution, which is suitable for Ge systems.
For the Li-glass system, which has a fast response signal
output, CAEN v1720 12-bit 250-MHz charge-sensitive
ADCs are prepared. Optical link connections are used
for data transfer from ADC boards to PC using CAEN
A3818 PCI express board. The maximum data transfer
rate was about 80 MB/s/fiber.
3. DAQ system performance
Test of the new DAQ system was performed using
standard γ-sources and the ANNRI beamline. Figure 1
shows the Ge detector energy resolution dependency
on the shaping time setting, as tested by using 60Co standard γ-ray source. Keeping shaping time at 4 μs, a 2.7 keV
FWHM for a 1332 keV γ-ray was achieved. Moreover, 5 keV
FWHM was achieved even if the shaping time was only
1 μs. In the current DAQ system, the live time was about
60% for a 100 kcps event rate. With the new DAQ system,
90% live time for 100 kcps event rate was achieved. The
integral nonlinearity was also checked by using 152Eu
standard γ-ray source and 27Al(n,γ)28Al reaction in ANNRI.
When the energy dynamic range was set to 10 MeV, anonlinearity in the order of 0.3 keV was achieved.
81Neutron Science

MLF Annual Report 2014

Figure 1. The shaping time dependency of the energy resolution at 1332 keV in 60Co. Each point indicates the flat-top time of the
trapezoidal pulse shaping.

4. Development of total cross-section measurement system
Measurements of capture cross sections of Minor
Actinides (MAs) have been performed at ANNRI to improve the reliability of the cross section data for MAs.
However, capture measurements are not sufficient
to determine the resonance parameters accurately,
and total neutron cross-section measurements are required. Therefore, we are promoting the developmentof a technique to obtain total neutron cross sections
at ANNRI with Li-glass neutron detectors and the new
DAQ system, which is still in progress. The purpose of
the study is to obtain accurate resonance parametersof MAs.
The neutron total cross-section measurementfor 197Au was performed by the time-of-flight (TOF)
method with the Li-glass neutron detectors and the
new DAQ under development for the Li-glass detector.
Two types of Li-glass detectors were utilized for total
cross-section measurements. A GS20 6Li-glass detector
manufactured by OKEN with dimensions of 10 cm x 10
cm and thickness of 1 cm using enriched 6Li (6Li>90%)
was used to obtain transmission neutron TOF spectra.
Neutrons are detected by the 6Li-glass detector via the
6Li(n,α)3H reaction. Furthermore, we used a GS-30 7Liglass detector manufactured by OKEN with dimensionsof 10 cm × 10 cm and thickness of 1 cm depleted in 6Li(7Li>99.99%) in order to evaluate the background except for neutrons from neutron TOF spectra measured
with the 6Li-glass detector. The 6Li-glass detectors wereplaced in a borated polyethylene shield to reduce thethermal neutrons moderated by the structural material
in the experimental area. The distance between theseLi-glass detectors and the neutron source was 29 m.
Signals from the 6Li-glass detector were amplified with
the ORTEC 474 timing filter amplifier, and the TOF and82

the pulse height of each event were recorded event-byevent in a list-data format file with the DAQ.
Gold-197, which is a monoisotopic nuclide, has superior chemical stability, and the precise resonance parameters of 197Au are well known, so that 197Au is used
to validate experimental setup and data analysis. The
197Au sample (purity 99.99%) with diameter of 9.0 cm
and thickness of 1.0 mm was placed at the middle collimator. The distance between the neutron source andthe sample was about 15 m. The neutron beam was collimated by the X-stage and rotary collimators located at
an upstream side of the experimental area of the ANNRI
so that the size of the neutron beam becomes smaller
than that of the Au sample. The transmitted neutrons
were measured by the 6Li-glass detector.
We repeated the measurements of the 197Au sample (197Au run) and with no sample (blank run) to obtainthe neutron transmission ratio. A Pb filter with a thickness of 3.75 cm was used to reduce the dead time of the
Li-glass detector caused by intense gamma flash fromthe spallation neutron source. Neutron notch filters ofnatMn, natCo, natIn and natAg were utilized to estimate thebackgrounds due to frame overlap neutrons and gamma-rays from the TOF spectra obtained by the 6Li-glass
detector by the black resonance technique. Moreover,
we carried out the measurements of the background byusing the 7Li-glass detector.
In the beginning, dead time corrections were madefor TOF spectra assuming that the DAQ has a fixed deadtime of 750 ns for each signal. The backgrounds of the
TOF spectra of 197Au and blank runs were estimated andsubtracted, and the net TOF spectra were obtained.
Neutron beam intensity determined by the numberof proton beam pulses and proton beam power wereused for normalization of the background subtraction. Finally, total cross sections of 197Au were derived

MLF Annual Report 2014by using the net TOF spectra of 197Au and blank runs.
Figure 2 shows the preliminary results. In the thermalenergy region, the results are in agreement with theevaluation of JENDL-4.0 [2]. At the 4.9 eV resonance of
197Au, cross section data is not available because transmitted neutrons equaled 0.

Figure 2. Neutron total cross sections of 197Au in the neutronenergy region from 10–2 to 103 eV. The red points
indicate present results. The black line indicatesevaluated values of JENDL-4.0.

Neutron Science

5. Future Plans
A new DAQ system and new total neutron crosssection measurement system have been developed at
ANNRI. The latter meets the demanded performance
specifics that measurements of gamma-ray capture
cross sections can be measured fine energy resolution by the Ge detectors and total neutron cross sections can also be obtained by the 6Li-glass detector.
Measurements of the neutron capture and total neutron cross-sections of 241,243Am are planned.
The author would like to thank the accelerator
and technical staff at J-PARC for operation of the accelerator and the neutron production target and for theother experimental supports. Present study includes
the result of “Research and Development for accuracy
improvement of neutron nuclear data on minor actinides” entrusted to the Japan Atomic Energy Agency by
the Ministry of Education, Culture, Sports, Science andTechnology of Japan (MEXT).
References[1] http://www.caen.it/[2] JENDL-4.0 data file for 197Au (MAT = 7925), evaluated by Iwamoto N (2010).

K. Terada and T. Nakao
Nuclear Data Center, Nuclear Science and Engineering Center, JAEA

83

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Present Status of BL05 (NOP)
1. Introduction
BL05 (NOP) is a beamline designed to carry out
fundamental physics experiments using neutrons. The
beamline is divided upstream into three branches to
conduct in parallel different experiments [1, 2]. The
present status of the ongoing experiments at BL05
(NOP) will be reported.
2. Measurement of the neutron lifetime
A neutron decays into a proton, an electron, and an
antineutrino. The lifetime is an important parameter for
the unitarity of the CKM matrix or primordial big bang
nucleosynthesis. However, the recently reported values
for the neutron lifetime deviate significantly from thesystematic errors claimed and require improvement.
An experiment to measure the neutron lifetime witha pulsed beam is ongoing at BL05 (NOP). The lifetime
is measured as the ratio of the electron events to the
3He(n,p)3H events caused by precisely doped 3He gas
using a time projection chamber (TPC) [3].
The TPC was improved in May, 2014. The inner surface of the TPC was lined by 6LiF/PTFE tiles to capture
scattered neutrons without gamma rays. The tiles werecovered with a PTFE sheet to suppress the ions causedby neutron captures. In the commissioning run of 2012,
contamination events due to 6Li(n,t)4He by leaks fromgaps of PTFE sheet were observed. By improving thecoverage of the PTFE sheet, we reduced successfully
the contamination (see Figure 1, left). In 2012, the energy resolution of the TPC was getting worse with theelapsed time. We found it was due to charging up andsolved the problem by setting electrodes to define voltages instead of the charging up material. As a result, theenergy resolution of the X-ray from 55Fe was improved
Before Improvement

After Improvement

Figure 1. Figure 1: Before and after improvement of the TPC.
Contamination due to 6Li(n,t)4He disappeared (left),and gained stability measured by 55Fe (right), respectively.

84

from ~20% to 12%, and remained stable in time (seeFigure 1 Right).
Physics data were taken for about 2 weeks by the
improved TPC. The data are under analysis by using
Monte Carlo simulation. In Figure 2, the track length
spectra of the beta decay candidates are shown withsimulations. The simulation reproduced the signals well(χ2/ndf < 2).
X distanceY distance

Figure 2. Spectra of the beta decay candidates with Monte
Carlo simulation. The X distance was calculated by
the number of hit wires. The Y distance was calculated by the drift time.

3. Ultracold neutron production by Doppler shifter
Ultracold neutrons (UCNs) with energy of less than~250 neV (velocity of 6.8 m/s), are utilized for various
precision measurements in fundamental physics. In order to develop and test UCN optical devices, a Doppler
shifter was installed to provide UCNs on BL05 (NOP)
beamline. The Doppler shifter reflects very cold neutrons (VCNs) with velocity of ~136 m/s by a moving mirror with 68 m/s and produces neutrons with less than
20 m/s.
The reflected neutron intensity at an extraction
port on the top was 410 cps at the 1-MW equivalentbeam power [4]. The reflected neutron flux was compared with a Monte Carlo simulation, which is shownin Figure 3. The measured and calculated spectra werein good agreement. The UCN intensity and peak UCN
density are estimated as 160 cps and 1.4 /cm3 according
to the simulation [4].
An additional port was set up at the side of the
Doppler shifter. A UCN storage vessel to study reflectivity of UCN on surfaces was installed (Figure 4). UCN
storage experiment will be performed.

MLF Annual Report 2014

Neutron Science

Figure 3. Measured (dotted) and calculated (solid) longitudinal UCN wavelength spectra of Doppler shifted
neutrons. The dashed line shows that of UCN,
whose total velocity is less than 6.8 m/s [4].

Figure 4. Additional side UCN port (left) and a UCN storage
chamber assemble with the Doppler shifter (right).

References[1] KENS Annual report 2014.
[2] K. Mishima, Neutron network news (Hamon), vol25,
No2 (2015) 156-160.
[3] Y. Arimoto, N. Higashi, Y. Igarashi, Y. Iwashita, T.
Ino, R. Katayama, R. Kitahara, M. Kitaguchi, H.
Matsumura, K. Mishima, N. Nagakura, H. Oide, H.
Otono, R. Sakakibara, T. Shima, H.M. Shimizu, T.
Sugino, N. Sumi, H. Sumino, K. Taketani, G. Tanaka,

M. Tanaka, K. Tauchi, A. Toyoda, T. Tomita, T. Yamada,
S. Yamashita, H. Yokoyama, T. Yoshioka, Nuclear
Instruments and Methods in Physics Research A,
799 (2015) 187-196.
[4] S. Imajo, K. Mishima, M. Kitaguchi, Y. Iwashia, N. L.
Yamada, M. Hino, T. Oda, T. Ino, H. M. Shimizu, S.
Yamashita, R. Katayama, Progress of Theoreticaland Experimental Physics (PTEP),accepted.
http://arxiv.org/abs/1507.07223v3.

K. Mishima1,2 on behalf of NOP collaboration
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK85

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MLF Annual Report 2014

BL06: Commissioning Status of VIllage of Neutron
ResOnance Spin Echo Spectrometers (VIN ROSE)
1. Introduction
The neutron spin echo (NSE) technique is an essential spectroscopic method, which at present time hasachieved the highest neutron energy resolution. NSEwith a pulsed neutron source makes it possible to scanvery efficiently a wide spatiotemporal space. Kyoto
University and KEK have been installing jointly two
types of NSE spectrometers at BL06 since 2011, that is,a neutron resonance spin echo (NRSE) instrument and a
modulated intensity by zero effort (MIEZE) instrument.
One of the characteristics of the instruments is the useof resonance spin flippers that make it possible to installcompact and multiple spectrometers in a limited space.
The beam line has been named “VIN ROSE” (VIllage of
Neutron ResOnance Spin Echo spectrometers), which
will spawn a new field of spectroscopic methods [1].
Figure 1 shows the schematic top view and a recent
photo of BL06.

which were held in the precise positions and covered byiron shields to reduce the dose level. The spectra at theguide-end positions were measured by a 3He neutron
beam monitor with a borosilicate glass plate as an attenuator. Figure 2 shows the measured and calculated
neutron fluxes. Both the coefficient of attenuation forborosilicate glass and the wave-length dependent neutron detection efficiency for the monitor were corrected. In the case of NRSE, a very good agreement (95%)
was achieved, on the other hand, the agreement for
MIEZE was 56% due to the disagreement mainly in the
shorter wavelength range. At this moment, we are carefully considering the reasons that may originate fromthe misalignment of the mirrors, their deflection, etc.

Figure 1. Top: a recent picture of BL06. Bottom: schematic
top view of the MIEZE and NRSE beam lines at BL06.

2. Commissioning Status at BL06
BL06 has been allowed to accept neutron beams
since April, 2014. After that, the performance of theinstalled neutron guides had been tested with several
methods. All the supermirrors for the guides (Qc = 2.5
and 3 for NRSE and MIEZE, respectively) were made at
KURRI by using the ion beam sputtering machine [1, 2],
86

Figure 2. Measured (solid line) and calculated (dashed line)
absolute neutron fluxes of NRSE (top) and MIEZE(bottom).

After the investigation of the neutron guide performance, we installed the components (a polarizer, two
resonance spin flippers, and an analyzer) in MIEZE to observe the neutron spin echo signals. The combination

MLF Annual Report 2014

Neutron Science

Figure 3. Left: (a) the measured TOF-MIEZE signal with an effective frequency of 200 kHz, (b) the TOF-MIEZE signal between 25 and25.1 ms, (c) power spectrum of the TOF-MIEZE signal by Fourier transformation. Right: (d) picture of the MIEZE spectrometer at BL06 VIN ROSE.

of MIEZE and time-of-flight (TOF) is a quite new method, and the related previous studies were just tentative [3, 4]. Therefore, the quantitative verification of
TOF-MIEZE was necessary and expected. We were able tomeasure successfully TOF-MIEZE signals with several different conditions. The measured TOF-MIEZE signal with
an effective frequency of 200 kHz is shown in Figure 3.
The time range of the TOF signal is between 0 and 80 ms
due to the double frame (12.5 Hz) operation of the disk
chopper. The acceptable neutron wavelength was limited by the opening section of the chopper. Very clear oscillation can be observed for the wide wavelength band(from 4 Å to 12 Å). Fourier analysis of the signal confirms
an exact 200 kHz oscillation, see Figure 3c.
As a next step, now we are investigating the detailed characteristics of TOF-MIEZE.
3. Summary
After a brief introduction, the current status of BL06

VIN ROSE was described. In FY2014, we were able toobserve the TOF-MIEZE signal successfully. Now we areproceeding with further commissioning for both MIEZE
and NRSE. Some standard experiments with MIEZE may
start in FY2015.
References[1] M. Hino, T. Oda, M. Kitaguch, N. L. Yamada, H.
Sagehashi, Y. Kawabata, and H. Seto, Physics Procedia
42, (2013) 136.
[2] M. Hino, H. Sunohara, Y. Yoshimura, R. Maruyama, S.
Tasaki, H. Yoshino, and Y. Kawabata, Nucl. Inst. Meth.
A 529, (2004) 54.
[3] M. Bleuel, M. Bröll, E. Lang, K. Littrell, R. Gähler, andJ. Lal, Physica B 371, (2006) 297.
[4] G. Brandl, J. Lal, J. Carpenter, L. Crow, L. Robertson,
R. Georgii, P. Böni, and M. Bleuel, Nucl. Inst. Meth. A
667, (20012) 1.

H. Endo1,2, M. Hino3, T. Oda4, N. L. Yamada1,2, H. Seto1,2, and Y. Kawabata3
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3Kyoto
University Research Reactor Institute; 4Departmente of Nuclear Engineering, Kyoto University Graduate School of Engineering

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MLF Annual Report 2014

Status Report for BL08 SuperHRPD

2. New detector system with an 8-mm diameter position sensitive detector
Initially, we installed 1/2-inch diameter position sensitive detectors (PSDs) that had been used at the KENS
facility of KEK since the initial budget was limited andthe development of the high spatial-resolution detector system was stopped. The imposed limit reduced the
instrumental resolution compared with the original design. Then we developed a new detector system basedon 8-mm diameter PSDs and managed to improve theresolution as shown below. The 16 PSDs of 8 mm in diameter were assembled together into one unit and an
amplifier circuit was connected to each PSD. In the newdetector system, 8 amplifier circuits were built into one
application specific integrated circuit (ASIC) chip andthis contributed to a more compact circuit (Fig. 1).

Figure 1. The conventional amplifier circuit (left) and the advanced one with an ASIC chip (right); the 16 amplifier circuits are implemented within two ASIC chips.

88

A new detector system installed at the backwardbanks in FY2013 has improved the overall resolution
from Δd/d = 0.1% to 0.08%. The best resolution of
0.04% was attained by using limited number of detectors located at high angle as well as narrowing down
the width of the beam as shown in Fig. 2. All detectorsof the backward bank were replaced with this new detector system, and have been routinely used to conduct
all measurements in FY2014. The Rietveld analyses havealready been successfully applied to data obtained
from the new detector system.
2500

2000

intensity / arb.unit

1. Introduction
SuperHRPD is the world’s highest resolution neutron powder diffractometer. SuperHRPD is expected to1) detect tiny distortion never detected before in thefield of strongly correlated systems, multiferroics, magnetic materials, etc., 2) attain high precision structure
analysis in energy materials, and 3) develop the structure science of hybrid materials, supermolecules, pharmaceuticals, etc. [1-3]. In the S-type project in 2014, we
continued to develop SuperHRPD as well as Z-Code, apowder diffraction data analysis suite, and worked on
various scientific topics including the Elements Strategy
Initiative of MEXT and the RISING project of NEDO (TheNew Energy and Industrial Technology Development
Organization).

NIST Si Powder SRM640d
2θ > 170° part
fitting function : asymmetric pseudo-Voigt
Resolution Δ d/d = 0.0409406(8)%

1500

1000

500

0
77.8

77.9

78.0

78.1

78.2 × 103

tof / μsec

Figure 2. Neutron diffraction pattern of a NIST Silicon powder sample (6 mm diameter) with 8 mm PSD. The
peak fitting result is obtained by an asymmetricpseudo-Voigt function.

3. Scientific topics
One of the scientific highlights was achieved by extracting precise structure factors using SuperHRPD [4].
Among the 4d transition metal oxides, SrRuO3 is known
to be a rare ferromagnet with Tc = 165 K, while CaRuO3
with the same structure shows nonmagnetic characterin the whole temperature range. SrRuO3 also has otherpeculiar and unexplained behaviors; one is a negative
thermal expansion below Tc, and the other is the failureof the Glazer structural description. In the Glazer description, which assumes a simple octahedron rotation,
the a axis is always shorter than the b axis in a distorted
ABO3 perovskite with Pbnm (a−a−c+; ‘−’ and ‘+’ represent the out-of-phase tilting and the in-phase tiltingof neighboring octahedrons, respectively). This rule isfound to hold for most orthorhombic perovskite compounds, with a few exceptions such as SrRuO3, whose aaxis is longer than its b axis.

MLF Annual Report 2014

Although tiny atomic structure changes below Tc
had not been detected in previous neutron diffraction experiments, SuperHRPD gave us precise in-plane
deformation of the RuO6 octahedra and structuralevidences for a negative thermal expansion and nonGlazer like distortion.
Below Tc, the average bond length <Ru–O> ofSrRuO3 obtained using SuperHRPD is ‘increased’ by aslittle as 0.0005 Å (such small distortion could not be
detected previously). In contrast, <Ru–O> of CaRuO3shows ‘decrease’ by an ordinary thermal expansion behavior at a low temperature, and <Mn–O> of
La0.75Ca0.25MnO3 shows some ‘decrease’ by 0.005 Å (tentimes of SrRuO3) upon entering its ferromagnetic state.

Figure 3. Glazer tilting description (Pbnm, a–a–c+). Mean
<Ru-O> and <Mn-O> bond of itinerant ferromagnetic SrRuO3, paramagnetic CaRuO3 and CMR
La0.75Ca0.25MnO3.

Neutron Science

These differences in the behaviors of the bond lengths
provide clear experimental evidence that a different
mechanism of ferromagnetism is at work for SrRuO3 as
opposed to La0.75Ca0.25MnO3. It is natural to think that anincrease in <Ru–O> at low temperature could make 4dbands of Ru localized. In fact, the calculated bandwidth
using an empirical formula shows temperature-induced
narrowing of the Ru 4d bands for SrRuO3, in contrast to
CaRuO3 and La0.75Ca0.25MnO3. So it is speculated that theferromagnetism in SrRuO3 is induced by the localizationof the Ru 4d bands.
References[1] T. Kamiyama and K. Oikawa, Proc. of ICANS-XVI,
Deusseldorf-Neuss, Germany, May 12-15 (2003) 309.
[2] S. Torii, M. Yonemura, Surya Panca Putra Y T, J.
Zhang, P. Miao, T. Muroya, R. Tomiyasu, T. Morishima,
S. Satoh, H. Sagehashi, Y. Noda and T. Kamiyama, J.
Phys. Soc. Jpn. 80 (2011) SB020.
[3] S. Torii, M. Yonemura, Y. Ishikawa, P. Miao, R.
Tomiyasu, S. Satoh, Y. Noda and T. Kamiyama,
Journal of Physics: Conference Series 502 (2014)
012052.
[4] S. Lee, J. R. Zhang, S. Torii, S. Choi, Deok-Yong Cho,
T. Kamiyama, Jaejun Yu, K. A. McEwen and Je-Geun
Park, J. Phys.: Condens. Matter, 25 (2013) 465601.
[5] M. Hiraishi, S. Iimura, K. M. Kojima, J. Yamaura,
H. Hiraka, K. Ikeda, P. Miao, Y. Ishikawa, S. Torii, M.
Miyazaki, I. Yamauchi, A. Koda, K. Ishii, M. Yoshida, J.
Mizuki, R. Kadono, R. Kumai, T. Kamiyama, T. Otomo,
Y. Murakami, S. Matsuishi & H. Hosono, Nature Phys,
10 (2014) 303.

S. Torii1,2, P. Miao1,2, S. Lee1,2, M. Yonemura1,2, and T. Kamiyama1,2
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK

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Development of an Advanced Special Neutron Powder
Diffractometer under Extreme Environment for Materials
1. Introduction
Batteries are a very important technology because
compact and wearable devices such as laptop computers and mobile phones, which work in an environment that lacks power, need mobile energy storages.
Additionally, high performance batteries are necessary
for larger devices, such as hybrid vehicles (HV) and pure
electronic vehicles (EV). Those vehicles are designed
to reduce the consumption of fossil fuels and advancethe transition to a low carbon society. The lithium-ion
battery is one of the most promising battery systems asenergy storage for both small and large cells. However,with the lithium-ion battery there are still challenges tobe resolved regarding its cyclic life and high temperature use. The capacity of that type of battery is also limited and needs to be improved.
The lithium-ion battery works through the lithium
ion transfer between cathode and anode. The reactionsof both electrodes are based on the de/intercalationof lithium ions from/into the materials of electrodes.
When the lithium ions intercalate into materials, thecrystal structure is changed. The information of thestructural changes and the location of lithium ions in
the crystal structure lead to improvement of the present lithium-ion battery and the invention of an out-ofthe-box battery.
In order to clarify at an atomic level the structuresof cathode, anode and the interface between electrodeand organic electrolyte, a new neutron powder diffractometer, SPICA, has been designed and constructed as
one of the state-of-the-art measurement apparatuses.
Compared to the X-ray, the neutrons are well known to
be a powerful probe to get information about the location and movement of light elements such as hydrogenand lithium atoms. Therefore, the advantage of the neutron diffraction will allow us to expand our knowledge
about the location and movement of lithium ions, aswell as the changes of the atomic arrangement in thecathode, anode and the electrolyte solution.
2. Present Status
In a previous S-type project, a new special environment diffractometer, SPICA was designed andconstructed on BL09 in J-PARC/MLF. In the new S-type
project (2014S10), structure changes in variety of charge
and discharge rates will be collected and analyzed to90

determine the reasons for the batteries’ deteriorationand find out the underlying issues.
Typical examples of in operando measurement
for a commercialized Li-ion battery (LIB) in low rate ofcharge and discharge were carried out in the stage ofthe commissioning. Those data revealed that SPICA had
a high potential of in operando measurement.
Figure 1 shows the discharge rate dependence ofstructure changes in anode materials. These diffraction
patterns show 00l diffraction of the graphite. Stage 1,
2, 3, 4 are different stacking structures of lithium in thegraphite layers respectively. Stage 1 and 2 coexisted inboth discharge rates. However, the coexistence regionsin the low-rate discharging were narrower than in thehigh-rate one. This discharge rate dependence might
indicate the inhomogeneous reaction on the large areaof anode sheet or/and slow conductivity of Li-ion in
the graphite. Because the slurry of the anode material,
which was made from graphite, PVDF (PolyVinylidene
DiFluoride) and NMP (N-Methyl-2-Pyrrolidinone) coated by just putting over using scrapers on power collector film, the high and low reactive region might coexist
on the electrode sheets.

Figure 1. The discharging rate dependence of the structurechanges of the anode material, graphite in discharge processes. Those diffraction patterns wereobtained by in operando measurements on SPICA.

Figure 2 shows the structure change of graphite inhigher discharge rate (2C). The white line indicates theborder of stopping the discharge. After the discharging
stopped, the structure still continued changing. Stage 1

MLF Annual Report 2014

Neutron Scienceand 2 also coexisted at the same low rate. Stage 3 also
appeared from the early stage of the discharge process.
The graphite phase appeared before Stage 4. After thedischarging stopped, the graphite peak disappearedand Stage 4 appeared simultaneously. In discharge in
2 C rate, the lithium ions still remained in the anodes.
Therefore, the relaxation behavior might be observed
because some concentration distributions of lithium
ions were formed in the high rate discharging.
3. Conclusion
The 18650-type lithium-ion batteries were measured using in operando technique. From those data,
the dependence on the charge–discharge rate was determined. The relaxation reactions in the anodes werequite different by charge–discharge rate. To find out
the issues causing degradation and unsafety, the relationship between reaction in batteries and structurechanges of electrodes will be determined in a variety ofcharge-discharge conditions.

Figure 2. The structure changes of anode material, graphite
in 2 C rate charge process.

Acknowledgements
We would like to appreciate Mr. K. Muroya and
Mr. S. Sugai for their technical support in constructing
the SPICA diffractometer. This work was supported by
the Research and Development Initiative for Scientific
Innovation of New Generation Batteries (RISING)
project of the New Energy and Industrial Technology
Development Organization (NEDO).

M. Yonemura1,2, T. Kamiyama1,2,3, K. Mori4, T. Fukunaga4, Y. ishikawa1, S. Torii1,2, R. Tomiyasu1, K. Kino5, T. Naka6, M. Morishima6,
S. Shiotani6, S. Taminato7, M. Hirayama7, R. Kanno7, Y. Onodera4, Y. Ukyo6, H. Arai6, Y. Uchimoto8, and Z. Ogumi6
1Institute of Materials Structure Science, KEK; 2Neutron Science Section, Materials and Life Science Division, J-PARC center; 3Neutron
Science Section, Materials and Life Science Division, J-PARC Center; 4Research Reactor Institute, Kyoto University; 5Hokkaido University;
6Ofﬁce of Society-Academia Collaboration for Innovation, Kyoto University; 7Interdisciplinary Graduate School of Science and Engineering,Tokyo Institute of Technology; 8Graduate School of Human and Environmental Studies, Kyoto University

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BL10: NOBORUIn FY 2014, 23 general use proposals were carriedout at NOBORU, but some of them have not been completed due to the fire in the MLF on January 16, 2015.
This year, we measured the neutron flux with highpower proton beam study up to 0.53 MW. Figure 1
summarizes ratio of the neutron flux vs. proton beam
power measured at BL10. Each neutron flux was integrated from 1 meV to 100 meV. The result indicatedthat the neutron intensity was almost proportional tothe proton beam power but depended on the proton
beam profile, because the proton beam profile differedin both measurement years. This study will continue up
to the 1 MW proton beam operation.

sample used in the imaging experiment. Figure 2 showsa high-resolution transmission image of four pieces ofcast duplex stainless steel using the μPIC detector andthe fitting result of transmission data of a small part ofsample no.1. The fitting result suggests the existence ofa strong texture structure in the BCC phase. The same
sample was measured by diffraction method at theBL10 using PSDs. Figure 3 shows the diffraction pattern
and the textured Deby-Scheller ring on a PSD. The rightfigure shows a strong BCC (110) texture pattern as predicted by the Bragg edge analysis.

Figure 2. Transmission image of wavelengths of 3.3–3.6 Åcollected using the μPIC detector (left); Fitting of
the Bragg-edge spectra of the position A in specimen no. 1 using RITS code (right) [1].

Figure 1. Ratio of intensity vs. proton beam power.

[Feasibility study on Bragg edge imaging and diffraction experiment using the same sample]
Energy resolved neutron imaging has been developed at BL10 since 2008. Now we have some characteristic 2D counting-type detectors. In particular,
the micro-pixel chamber (μPIC) detector and the Gas
Electron Multiplier (GEM) detector show good spatial
resolution and high-count rate capability, respectively.
This year we purchased 1D-PSDs for diffraction measurement to obtain complementary information of the

Figure 3. Pawley fitting pattern of the diffraction data of sample no.1 (left) and the textured Deby-Scheller ringon the PSD (right).

Reference[1] Y. Su et al., JPS Conf. Proc. 8 031015 (2015).

K. Oikawa and M. Harada
Neutron Science Section, Materials and Life Science Division, J-PARC center92

MLF Annual Report 2014

Neutron Science

BL11: Structure Analysis of Crystals and Amorphous
Solids at 18 GPa with Paris-Edinburgh Press
1. Introduction
The compression of materials induces changes intheir physical properties. To understand that mechanism, it is essential to explore their structure. Neutron
diffraction is effective in revealing structures of materials including light elements, such as hydrogen and oxygen. In particular, the in-situ observation of structures
under high pressures is important because the structure appeared at high pressures sometimes reverts tothe original one after the release of pressure.
In past research in Japan, the routinely accessible pressure of in-situ observation has been limited
to about 3 GPa, although it has reached up to 30 GPa
at other research facilities around the world. This year
we tried in-situ neutron diffraction at 18 GPa by using
Paris-Edinburgh press (PE press) [1, 2].
Generally, the quality of the diffraction patterntaken at such pressures is not good due to the contamination of Bragg peaks from the high-pressure anvils.
PLANET [3] is equipped with radial collimators which
can eliminate them. By coupling the radial collimatorsand the PE press, we managed to obtain clear patterns
and analyzing structures of crystals and amorphous solids precisely at 18 GPa. Here, we report the experimental details and share several examples.
2. Method
The diffraction geometry used in the experiments
is shown in Fig. 1. The sample (typically 4 mm in diameter and 3.1 mm in height) is compressed by a couple ofsintered diamond anvils. The press is placed at sample

Figure 1. Diffraction geometry employed in the in-situ neutron diffraction experiments using Paris-Edinburgh
press.

position with the compression axis parallel to the incident beam. Neutrons scattered by the sample are detected with two 90° banks. The incident collimator ofboron nitride with a hole of 4 mm defines the neutron
beam introduced into the sample and the radial collimator with a gauge length of 1.5 mm along the beam
direction eliminates the scattering from the anvils. This
setup enables us to obtain signals exclusively from thesample over scattering angles of 90°±3.7° horizontallyand 0°±34.6° vertically.
3. Example
Application to crystalline materials
To investigate the pressure response of hydrogenbond in the hydrous mineral δ-AlOOH and its D/H isotope effect, we performed neutron diffraction experiments at pressures up to 18.2 GPa. The sample was
loaded into a TiZr gasket together with pressure-transmitting medium of methanol-ethanol mixture and compressed with a PE press. The initial volume of the sample
chamber was 26 mm3. The booster focusing mirror wasused to increase the beam flux. Above 10 GPa, a slightbroadening of the diffraction peaks was observed, from
0.7% in Δd/d at ambient condition to 1.08% at 17.4 GPa
because of the non-hydrostatic stress caused by the solidification of the pressure transmitting medium.
Figure 2 shows the observed diffraction pattern of
δ-AlOOD at 17.4 GPa and the results of Rietveld fitting.
The exposure time of 4 hours at 17.4 GPa at the accelerator power of 290 kW was sufficient to refine the structure. The transition from the P21nm phase to a Pnnm one

Figure 2. Observed and calculated patterns of δ-AlOOD at
17.4 GPa. Tickmarks show the calculated peak positions of δ-AlOOD and the diamond that was usedas the anvil of the PE press.

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was observed at 12.1 GPa in δ-AlOOD. This pressure wasalmost the same as the condition at which the change
in compressibility was found previously. The result revealed that even small changes of the hydrogen position
by compression affect the bulk compression behavior.
Structure analysis of amorphous materials
We have investigated the structure of SiO2 glassat pressures up to about 17 GPa in order to reveal thecontraction mechanism and the possible existence offirst-order amorphous-amorphous transition underhigh-pressure condition.
The sample shaped into a form which fits into thedip on the anvil top (4 mm in diameter and 3.6 mm inheight) was placed between the anvils and compressed
to 17 GPa with no pressure transmitting medium. The
generated pressure was estimated from the pressureload curve checked prior to the experiments.
Figure 3 shows a set of raw data for three profiles(i.e. sample, vanadium and empty) taken with the PEpress. The exposure time for each pattern was typically
24 hours. It is clear that the Bragg peaks from the anvils

were hardly observed in any profile, thanks to the radialcollimator.
The data were analyzed with the Python code
“nvaSq” developed for structure analysis of disorderedmaterials at BL21 NOVA. Figure 4 shows the S(Q) obtained in this study, together with that below 10 GPa
in the previous study. The pressure dependence shows
marked changes in the raw-Q region reflecting thestructure of intermediate range order. On the other
hand, no significant changes were observed in thelong-range oscillation part reflecting the short-rangeorder. These observations are consistent with the previous view on the contraction of the SiO2 glass. The resultsof the detailed analysis will be published elsewhere.

Figure 4. S(Q) of SiO2 glass at pressures up to 17 GPa. S(Q)below 10 GPa was taken with six-axis press [4] andthat at 17 GPa was taken with PE press.

Figure 3. Raw data taken with the PE press (S; sample at
17 GPa, V: vanadium at 17 GPa, E: Empty: gasket
only at ambient pressure).

References[1] J. M. Besson et al., Phyica B 180-181, 907 (1992).
[2] S. Klotz et al., High Press. Res.24 219 (2004).
[3] T. Hattori et al., Nuclear Inst. and Meth. Phys. Res.,
A780 55 (2015).
[4] A. Sano-Furukawa et al., Review of Scientific
Instruments, 85, 113905 (2014).

T. Hattori1,2, A. Sano-Furukawa1,2, K. Funakoshi3, J. Abe3, and S. Machida3
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Quantum Beam Science Directorate, JAEA; 3Neutron R&D
Division CROSS-Tokai

1

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High Resolution Chopper Spectrometer at BL12
1. Introduction
The High Resolution Chopper Spectrometer (HRC)
is being operated at BL12 to study the dynamics in condensed matters with high resolutions using relatively
high energy neutrons. A research project using the HRC
is being conducted to observe a wide range of correlated electron systems. Based on the achievements in the
1st phase of our project (FY2009-2013), we will improve
the performance of the HRC in the 2nd phase startingfrom FY2014, in the following areas: (1) low angle detecting system for high energy experiments, (2) Fermi
choppers for higher resolution and lower backgroundin the high energy region, (3) sample environment
equipment, especially the superconducting magnet,(4) completion of installing detectors at high angles,and (5) computational environment for easy operationof experiments.
2. Instrumentation in FY2014
In the initial construction, 128 pieces of 2.8 m PSDs,
which are mounted into two detector banks, covered
φ = 3° - 42°. 64 pieces of 2.8 m PSDs are mounted oneach detector bank panel of 1.5 × 3 m2 with a vacuum
flange on the vacuum scattering chamber. 128 more
pieces of PSDs for another two detector banks werepurchased and mounted. These detectors cover φ =−30° - 60° at present.
We have a variety of sample environments: three
types of refrigerators – GM type, 3He sorption pumping type, 3He circulation type – and a superconducting
magnet.
The GM-type refrigerator is conventionally used
to cool the sample stably down to 4 K. This refrigerator shows a good cooling performance by improving
the radiation shielding, which is made of thin Al foil
and is in contact with the cold head. Sample temperature as low as to 2.5 K and heat-up rate of 26 μK/minon the sample have been confirmed, as shown in Fig. 1.
A temperature sensor with fine calibration is used at
the sample, and another one with rough calibration isat the cold head. This may cause higher than normal indication at the cold head for the best case indicated by“ike” and “masu”.
The lowest temperatures of 0.3 K and 0.6 K wereconfirmed for the 3He sorption pumping type refrigerator and the 3He circulation type refrigerator, respectively. For the 3He sorption pumping type refrigerator,
an outer vacuum chamber (OVC) was attached in orderFigure 1. Temperature variations at the sample can (top) andthe cold head of the refrigerator (bottom) before
and after the improvement of the radiation shielding on the GM-type refrigerator.

to separate the vacuum surrounding the sample fromthe vacuum scattering chamber and keep the lowest
temperature, and the goniometer was modified for theattachment. For the 3He circulation type refrigerator, an
OVC was mounted in the initial manufacture process. In
order to reduce the background noise from the OVC forthese refrigerators, an oscillating radial collimator was
introduced.
On HRC we also installed a superconducting magnet with performance of maximum magnetic field of
14 T and the lowest temperature of 0.3 K. We performed
the commissioning at the Guide Hall of JRR-3M, andconfirmed that it was successfully operated with the
maximum magnetic field of 14 T at the lowest temperature of 0.3 K. Then we moved the superconducting magnet to the HRC, and examined the maximum
magnetic field in the actual setup of the experiments.
We confirmed a maximum magnetic field of 10 T on the
HRC without any damage to the devices around thesample area (Fig. 2).
95

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MLF Annual Report 2014a mechanical booster pump for the vacuum scattering chamber, and two scroll pumps for the T0 chopper
and the guide tube. The turbo molecular pump for the
Fermi chopper was replaced.

Figure 2. Successful operation of the superconducting magnet with the application of magnetic field of 10 T at
the sample position of the HRC.

In the control software, the graphical user interface (GUI) for the Fermi chopper was improved. Also,
the software necessary to control the superconducting
magnet, such as that for monitoring the magnetic field
and the temperature and controlling the sample orientation, was installed.
In the analysis software, some algorithms were improved, such as for the alignment of the sample crystal,for plural runs, for extraction of event data at a specified
time range, and for masking unused detectors or detector pixels.
In the computer hardware, the network attachedstorage (NAS) was increased from 44 TB to 76 TB, and aworkstation (Dell Precision T7610) for the MSlice analysis was set up.
Because the phase control of the Fermi chopper issometimes unstable, the stability in the phase control
and the balancing of the magnetic bearing were investigated. However, we could not obtain conclusive results.
A regular maintenance was performed for some
vacuum pumps such as two sets of scroll pumps and3. Scientific Results
On the HRC, the following studies were conducted in this fiscal year: magnetic model in multiferroics
NdFe3(BO3)4 [1], crystal field excitations in breathing
pyrochlore antiferromagnet Ba3Yb2Zn5O11 [2], high energy excitations in itinerant antiferromaget γ-FeMn [3],ferromagnetic order in CePd2P2 [4], investigation of
stripe and over-doped checkerboard ordering in layered nickel oxide Nd2-xSr xNiO4 [5, 6], crystal electricfield excitations in filled skutterudite PrRu4P12 [7], spinand hole dynamics in carrier doped quantum Haldane
chain [8], intermultiplet transitions in filled skutterudite
SmFe4P12 [9].
References[1] S. Hayashida, M. Soda, S. Itoh, T. Yokoo, K. Ohgushi,
D. Kawana, H. M. Rønnow and T. Masuda, Phys. Rev.
B 92 (2015) 054402.
[2] T. Haku, M. Soda, M. Sera, K. Kimura, S. Itoh, T. Yokoo,
T. Masuda, in preparation.
[3] S. Ibuka, S. Itoh, T. Yokoo, Y. Endoh, unpublished.
[4] Y. Ikeda, H. Yoshizawa, S. Konishi, S. Araki, T. C.
Kobayashi, T. Yokoo, and S. Itoh, J. Phys.: Conf. Series592 (2015) 012013.
[5] Y. Ikeda, S. Suzuki, T. Nakabayashi, H. Yoshizawa,T. Yokoo, and S. Itoh, J. Phys. Soc. Jpn. 84 (2015)
023706.
[6] Y. Ikeda, S. Suzuki, T. Nakabayashi, H. Yoshizawa, T.
Yokoo, and S. Itoh, J. Phys. Soc. Jpn. in press.
[7] K. Iwasa, A. Yonemoto, S. Takagi, S. Itoh, T. Yokoo, S.
Ibuka, C. Sekine, and H. Sugawara, Physics Procedia,
in press.
[8] T. Yokoo, S. Itoh, S. Ibuka, H. Yoshizawa and J.
Akimitsu, J. Phys.: Conf. Series 568 (2014) 042035.
[9] S. Konno, A. Ssuzuki, K. Nihei, K. Kuwahara, D.
Kawana, T. Yokoo, S. Itoh, J. Phys.: Conf. Series 592(2015) 012029.

S. Itoh1,2, T. Yokoo1,2, T. Masuda3, H. Yoshizawa3, M. Soda3, Y. Ikeda3, S. Ibuka1,2, T. Asami3, R. Sugiura3, D. Kawana3, Y. Kawamura3,
T. Shinozaki3, and Y. Ihata4
1
Institute of Materials Structure Science, KEK; 2Neutron Science Section, J-PARC Center; 3The Institute for Solid State Physics, The Universityof Tokyo; 4Technology Development Section, J-PARC Center96

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BL14 AMATERAS
1. Introduction
2014 was the sixth year of operation of AMATERAS,
a cold-neutron disk-chopper spectrometer (Fig. 1). We
continued the user program steadily without any serious problems, as described below.

Figure 2. B4C liners (10 mm in the thickness) were inserted
in-side the get-lost tube of AMATERAS.

Figure 1. Photo of AMATERAS (May, 2014).

2. Instrumental activities
In JFY2014, we carried out the following main instrumental activities: installation of a top-loading-type
cryostat and increase of the shielding.
Since the beginning of the user program, AMATERAS
has been equipped with a bottom-loading-type closedcycle refrigerator (CCR) as a standard sample environment, which realizes low background due to a minimal
Al window. This cryostat does not have an outer vacuum
chamber to share the adiabatic space with the scattering vacuum chamber of the instrument, so it takes halfa day to change the sample. In order to reduce this timeand perform experiments more effectively, this fiscal
year a new top-loading-type CCR for users’ experiments
was installed on AMATERAS. In our commissioning, wemeasured the reduction of background from the CCR
and performed off-bench and on-beam operation. This
CCR enables us to change the sample within an hour.
AMATERAS has a stainless steel duct to receive thedirect neutron beam, called get-lost tube. We had a problem with high radiation level around the beam dump
due to the γ-ray yielded at the duct, then we needed totake some measures before increasing the beam power
to 1 MW. In JFY2014, we covered the inside of the get-losttube with 10-mm thick B4C to prevent neutrons from hitting the stainless steel directly (Fig. 2). Furthermore, 100mm thick iron shielding was added onto the beam dump
(Fig. 3). After these measures, the radiation level aroundthe beam dump was dramatically lowered.

Figure 3. Additional shielding on the beam dump of
AMATERAS.

3. User Program
The research fields of the proposals on AMATERAS
had vary widely. In the 2014A and 2014B periods, 16
general use proposals were accepted, and six proposals were listed on the reserved subjects. We accepted
two project use proposals as continuations from the2013 period, which are ‘Study of structure and electronic properties of functional materials at BL14’ (PI: T.
Masuda) and ‘Project research on structure and dynamics of protonic, superionic and amorphous functional
materials using AMATERAS’ (PI: Y. Inamura). Also, two element strategy use proposals, ‘In-situ Neutron Analysis
of Advanced Structural Materials in Elements Strategy
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MLF Annual Report 2014

Initiative for Structural Materials (ESISM)’ (PI: N. Tsuji)
and ‘Neutron-scattering research on element-strategy
project for electronic materials’ (PI: Y. Murakami) were
accepted. Unfortunately, due to problems with the neutron targets and the linac and the fire accident in MLF,
we could not finish 5 proposals (general use: 3, element
strategy use: 1, project use: 1) and it was decided totransfer them to the next year.
AMATERAS joined the MLF School for the first timein mid-December. Three students participated andstudied QENS measurement and analysis for room temperature ionic liquids (Fig. 4). From a curve fitting with ajump diffusion model consisting of three Lorentzian dynamical modes at several temperatures, they reduced
the diffusion constant of the energy width of eachcomponent and activation energy of slowest diffusion

mode. We hope the neutron experiment will become
one of the tools used in their research activity.
4. Other Topics
AMATERAS had interim assessment done by
the MLF Neutron Instruments Review Committees.
Achievements in hardware development, user programs and other activities for the last five years werereviewed through documents and interviews. We received very positive comments and recommendations
to continue our activities in the way we had performed
them before.
Dr. H. Nakagawa was awarded by the JapaneseSociety for Neutron Science (JSNS) for his work on the
study of DNA dynamics done on AMATERAS. His work wasalso covered in a press release issued on August 29, 2104.

Figure 4. Students set sample in cryostat in MLF School.

K. Nakajima, S. Ohira-Kawamura, Y. Kawakita, and T. Kikuchi
Materials and Life Science Division, J-PARC Center98

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Neutron Science

Upgrading of TAIKAN
1. Introduction
The small and wide angle neutron scattering instrument TAIKAN (BL15) has been developed and upgradedto analyze microstructures or hierarchical structures ofsubstances in various scientific fields precisely and efficiently with a 1 MW spallation neutron source in J-PARC.
In FY2014, further upgradings for low-q measurement
and high-q measurement were done.
2. Upgrading of for low-q measurement
A focusing-geometry SANS method is adopted forthe measurement in a q range of 0.0005 – 0.005 A−1. For
the method, beam focusing devices and an ultra-smallangle detector are used. Figure 1 shows the beam focusing devices installed in the beam line. The devices
are a quadrupole magnet to polarize a neutron beamand two sextupole magnets to focus the neutron beampolarized by the quadrupole magnet on the ultra-smallangle detector. The detector is a high-resolution scintillation detector with an active size of 5 inch in diameterand spatial resolution of about 0.5 mm. Figure 2 shows
the detector and neutron image data obtained by thedetector with a mesh cadmium plate. From the data
it was confirmed that the detector can give data withsmall distortion and is available for SANS measurement.

4. Future prospect
The evaluation of the focusing-geometry SANS system will be performed with the devices and the ultrasmall-angle detector after installation of neutron spin
flippers in FY2015. TAIKAN will be a small and wide neutron scattering instrument in name and in reality before
long.

Figure 1. Magnets developed for focusing-geometry SANS
measurement: (left) a quadrupole magnet, (middle)
the first sextupole magnet, and (right) the second
sextupole magnet.

Figure 2. (Left) a high-resolution 2D detector and (right) neutron image data obtained by the detector.

I(q)(arb. units)

3. Upgrading of for high-q measurement
A backward detector has been installed in TAIKAN.
The performance of the detector was evaluated with
CeO2 powder. Figure 3 shows diffraction data measured

with the detector. The diffraction data can be analyzed
well by the Rietveld method.

TOF(msec)
Figure 3. Diffraction data of CeO2 powder measured with a backward detector.

J. Suzuki1, S. Takata2, K. Ohishi1, H. Iwase1, T. Morikawa1, Y. Kawamura1, M. Sahara1, T. Hosoya2, Y. Inamura2, T. Ito1, T. Nakatani2,
T. Shinohara2, T. Oku2, K. Suzuya2, K. Aizawa2, and M. Arai2
1
Neutron R&D Division, CROSS-Tokai; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center99

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Development of Elliptic Focusing Mirror for Samplefocusing Neutron Reflectometry at BL16
1. Introduction
Neutron reflectometry (NR) is very useful for investigations of structures of surfaces and buried interfaces
composed of soft materials. SOFIA is a horizontal-type
neutron reflectometer constructed at Beamline 16 (BL16)of the Materials and Life Science Experimental Facility(MLF) of the Japan Proton Accelerator Research Complex(J-PARC) [1, 2]. Due to the high-flux beam of J-PARC, lessthan one hour is needed for taking a full Q-range dataand only a few seconds for a limited Q-range data in thecase of a sample with 3 inches (76 mm) in diameter; eventhough the beam power is still one-third of the planned
value, 1 MW. However, several hours are still needed for asmall sample such as 10 mm × 10 mm, which is a typicalsize of a sample for X-ray reflectometry.
In the near future we plan to install an elliptical focusing mirror as a further upgrade of the SOFIA reflectometer. The focusing mirror will enable us to illuminatea sample with a neutron beam with a large beam divergence. In the case of conventional double slit collimation, the optimal beam divergence decreases according
to the sample size. Hence, the focusing optics with themirror has an advantage on the beam flux especially forsmall samples. The planned specifications of the focusing mirror and detector are a beam size of 0.1 mm at asample position with divergence of 2.5 mrad.
In this report we cover the development of a prototype of a focusing mirror with an elliptic shape and theresult of a reflectivity measurement with the focusing
mirror performed at BL16.
2. Manufacture and ray trace simulation
We employed an aluminum alloy as a base plate forthe focusing mirror. First, the base plate was machinedwith a single diamond tool to produce a rough surface
shape, in which the surface follows the center part of anellipse with a long axis of 4300 mm and a short axis of
430 mm. Then, the plate was coated with nickel phosphorous by electroless plating process, and finished byan ultrahigh precision cutting (UPC) process. The surface was polished before coating the super mirror tocreate a smooth surface of less than 1 nm in root meansquare (RMS) roughness. The super mirror with the mvalue of 3 was deposited on the substrate using an ion
beam sputtering instrument at the Kyoto University
Research Reactor Institute [3]. Since the mirror size,
100

550 mm in length and 60 mm in width, was too large tocoat the super mirror, the mirror was divided into twopieces and assembled into one unit after the processes
above were completed.
Figure 1 shows a photo of the mirror and theshape and figure error measured by a contact typethree-dimensional coordinate measurement machine(Mitsutoyo Bright Apex 1230). Although the surface
follows an elliptic shape, there were slight figure deviations from the ideal shape. To evaluate the effect of the
figure error, we performed a ray trace simulation withthe shape measurement result. The size of the lightsource at a focal point was 50 μm; therefore, the beamfocused on the other focal point, that is, the sample
position, ideally should be the same size. However, thebeam size at the sample position by the simulation was
0.3 to 0.4 mm because of the figure error. This meansthat the minimum beam size focused by the mirror islimited by the figure error.

Figure 1. Photo and shape of the focusing mirror made ofaluminum plates.

Figure 2. Ray trace simulation using a figure error measured
with a three-dimensional coordinate measurement
machine.

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3. Results
With the focusing mirror, we performed the focusing experiment at BL16. Figure 3 presents the focal image at the sample position. The size of a neutron source,
slit aperture, was 50 μm as the simulation above andthe image of the simulation was well reproduced. The
full width at half maximum (FWHM) of the image was
evaluated to be 0.34 mm by the fitting with a Gaussianfunction.

Neutron Science

approximately 3 times larger than that without themirror (1.94 counts/pulse).

Figure 4. Reflectivity profiles taken with a double slit collimation and a focusing mirror.

Figure 3. Focal image of neutrons at a focal point with asource size of 0.05 mm.

Furthermore, we attempted to measure the neutron reflectivity using an optics with the focusing
mirror. The size of the neutron source and incident
angle of neutrons were 0.4 mm and 1.2° degrees,
respectively, in which the beam size in the traveling direction was 20 mm. The sample was a deuterated polystyrene thin film on a Si substrate with adiameter of 2 inches (50.8 mm). For comparison, we
also performed the reflectivity measurement using a
conventional optics with double slits. Figure 4 shows
the reflectivity profiles with and without the focusing
mirror, in which the profiles show good consistency.
One thing we should emphasize here is that the countrate with the focusing mirror (6.40 counts/pulse) is

4. Summary
Here, we reported the development of the focusing
mirror for the neutron reflectometer SOFIA. The mirror
is capable of focusing neutrons with a width of 0.34 mm
in FWHM. With this mirror, a reflectivity measurement
was carried out and the gain factor was approximately
3 in comparison with the conventional double slit collimation. We are now planning to fabricate a new focusing mirror, in which some critical processes we becameaware of by using the prototype mirror are modified todecrease figure errors for 0.1 mm focusing. As the gain
factor increases with the reduction of the beam size,
this mirror will enable us to measure smaller samples
more efficiently.
References[1] N. L. Yamada et al., Euro. Phys. J. Plus, 44 (2011) 9424.
[2] K. Mitamura et al., Polymer J., 45 (2013) 100.
[3] M. Hino et al., Nucl. Instr. and Meth. A, 797 (2015)
265.

N. L. Yamada1,2, T. Hosobata3, M. Hino4, S. Takeda5, J. Guo3, S. Morita6, T. Oda4, J. Kato3, Y. Yamagata3, and M. Furusaka5High Energy Accelerator Research Organization, Tokai, Japan; 2Japan Proton Accelerator Research Complex, Tokai, Japan; 3RIKEN Center
for Advanced Photonics, Wako, Japan; 4Kyoto University, Kumatori, Japan; 5Hokkaido University, Sapporo, Japan; 6Tokyo Denki University,
Tokyo, Japan

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BL17: Neutron Reflectometer SHARAKU
1. Introduction
Polarized neutron reflectometry is one of the powerful methods for studying the surface and interface
structure of magnetic materials. The polarized neutronreflectometer SHARAKU [1], named after the famous
Japanese ukiyo-e printer, was installed at BL17 as thesecond reflectometer of the MLF. SHARAKU was constructed in the beginning of 2012, and then we started
the commissioning and a portion of the user program.
Now SHARAKU is widely open to international users. In
this article, we cover the progress achieved in this fiscal
year.
2. Neutron polarization in weak magnetic field
Weak magnetic materials are widely used in electric and electronic devices, and are some of the mostinteresting targets for the polarized neutron reflectometer. Due to their low magnetic coercivity, theweak-magnetic-field polarization system should be
generated for their polarized neutron reflectivity analysis. In SHARAKU, the polarization system in a strong
magnetic field (10 kOe in a sample position) works well.
However, the polarization system in a weak magnetic
field is not enough to analyze weak magnetic materials.
Therefore, we installed some guide coils to connect theguide magnetic field before and after a sample position, and optimized their current values.
Figure 1 shows the time-of-flight (TOF) spectra
obtained with the polarized neutron analysis mode in
weak magnetic field (50 Oe in a sample position). The
spin states of incident and scattered neutrons wereselected to produce the non-spin-flip cross sections(R++(red) and R−−(green)) and the spin-flip cross sections(R+− (yellow) and R−+(blue)) as shown in Fig. 1. The flipping ratio (F) values were determined by the ratio of F+= R++/R+− or F− = R−−/R−+. It is clear that the neutron polarization was maintained in weak magnetic field, and its
mean flipping ratio of 50 Oe condition within the wavelength of 2.4 < λ (Å) < 8.4 was 51.8.
Since the mean flipping ratio of 10 kOe was 54.5,
it can be concluded that the magnetic field construction was sufficiently improved by this commissioning.
Further improvement in the lower magnetic field (<50 Oe) will be conducted in the future.
3. Development of the data analysis system
We have used the software Utsusemi [2] and BL17
original software to analyze the measured neutron TOF
102

Figure 1. TOF spectra obtained with polarized neutron analysis mode (above) and theflipping ratios (below) in
50 Oe condition.

Figure 2. TOF spectra obtained with polarized neutron analysis mode (above) and the flipping ratios (below) in
10 kOe condition.

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Neutron Science

Figure 3. Operation panels of the data reduction program. Upper left is a TOF data output program, lower left is a reflectivity calculation program, and right is a reflectivity data connection program.

data and to convert the TOF data into neutron reflectivity profiles, respectively. However, these data reduction
procedures are slightly complicated and it was difficult
to obtain and check the reflectivity profiles during measurement. Therefore, we had to improve this situation
by development of a new data analysis system.
In 2014, new data reduction, normalization, andsubtraction programs were developed and installedin SHARAKU. Figure 3 shows the operation panels of
the data reduction program. The TOF and reflectivity
profiles can be obtained by input of a run number andexperimental conditions, and these programs can show
reflectivity profiles on display even during measurement. Now, the data analysis system has been utilized
not only for data reduction but also for the on-timemonitoring system of reflectivity measurement.
References[1] M. Takeda et al., Chinese J. Phys. 50 (2012) 161.
[2] Y. Inamura et al., Proc. 19th Meeting on Int.
Collaboration of Advanced Neutron Sources (2010)10-01.

N. Miyata1, S. Kasai1, K. Akutsu1, M. Takeda2,3, D. Yamazaki3,4, K. Soyama4, J. Suzuki1, Y. Inamura3, and T. Nakatani3
Neutron R&D Division, CROSS-Tokai; 2Quantum Beam Science Center, JAEA; 3Neutron Science Section, Materials and Life Science Division,
J-PARC Center; 4Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center

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BL18: Current Status of SENJU
1. Introduction
SENJU is a TOF single-crystal neutron diffractometer designed for precise crystal and magnetic structure
analyses under multiple extreme environments such as
low-temperature, high-pressure and high-magnetic
fields, and also capable of taking diffraction intensities of small single crystals with volumes of less than
1.0 mm3 down to 0.1 mm3.
In 2014, we developed a cryostat for photo crystallography to enable in-situ light-exposure neutron
diffraction measurements, and upgraded the data visualization program to ease the development of a diffraction measurement strategy.
2. Development of a cryostat for photo crystallo-graphy
Photo-induced crystalline-state properties, suchas light-emission and magnetism of organic molecular
crystals, have been actively investigated because they
can derive new photo-functional organic materials. In
recent investigations of those molecular crystals, insitu light-exposure X-ray diffraction is one of the mostimportant techniques to determine the photo-induced
chemical species. On the other hand, neutron diffraction
is a powerful technique to observe hydrogen atoms,
which are difficult to observe by X-rays. If visible lightis induced in a closed-cycle cryostat and in-situ lightexposure neutron diffraction measurement of thosecrystals under low temperature becomes possible, wewill be able to trap the photo-induced metastable species produced by the proton transfer and determine
their structure including the transferred proton, whichis hard to determine by X-rays. Consequently, the researchers of photo-functional materials will obtain a
new powerful analysis technique.
In 2014, as shown in Figure 1, we developed a newclosed-cycle cryostat with 2-axe goniometer in which
visible white light can be induced to carry out an in-situ
single crystal neutron structure analysis of a photo-induced species in a single crystal on SENJU. The cryostat
is composed from a 4 K pulse-tube refrigerator, a fixedχ type 2-axe goniometer using piezo-rotators and an
optic fiber light guide. There are several service ports at
the interface between the vacuum part and the atmospheric part and a vacuum connector, in which the lightguide is embedded, is set on one of the service ports.
The forefront of the light guide is covered with superinsulation film and fixed on an optical port of the 4 K
radiation shield near the goniometer. Visible light is led
104

into the vacuum part of the cryostat through this lightguide and exposed to the sample crystal, as shown in
Figure 2. The Xe light source for the cryostat, MAX-303(ASAHI SPECTRA Co.), has some wavelength selecting
filters and the optimum wavelength region for each experiment can be chosen. The lowest temperature at the
sample position is 8 K without photo-irradiation, 11 K
with a 400 nm band-path filter, 18 K with a 400 nm longcut filter and 66 K with no filter.

Figure 1. Side view of the cryostat for photo crystallography.

Figure 2. Sample position of the cryostat.

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Figure 3. Screen of STARExplorer. The upper left window shows the reciprocal space and the colored dots indicate surveyed Bragg
peaks. The upper right window displays the goniometer angles.

3. Development of a new reciprocal-space visualization program “STARExplorer”
In a usual experiment at SENJU, diffraction imagesof one sample crystal are measured with several orientations of the crystal. Thus, visualization of “surveyed”
and “unsurveyed” reciprocal space is very importantto optimize the orientation of the crystal. Therefore, in
2014, we developed a new reciprocal-space visualization program called “STARExplorer”.
STARExplorer is a web-browser based program

written in JavaScript (WebGL), which works on Windows,
OSX and CentOS. It shows a 3D image of the surveyed
reciprocal space as shown in Figure 3 from a UB-matrix
and goniometer angles entered by a user. The 3D imageof the reciprocal space can be rotated and enlarged bymouse action.
4. User program
Seven general proposals were conducted in 2014A,
and five more in 2014B.

T. Ohhara1, R. Kiyanagi1, A. Nakao2, T. Hanashima2, K. Munakata2, T. Moyoshi2, and T. Kuroda2
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division CROSS-Tokai

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Status of TAKUMI (BL19)
1. Overview
The TAKUMI operation in JFY2014 was stable. The
user, project and instrumental programs were performed successfully. Also, several enhancements inboth the hardware and the software were performed,
and their details are described below.
2. Enhancement of the neutron detection bank
There is a pair of neutron detector banks (northand south detector bank) in TAKUMI for simultaneous
detections of two orthogonal strains. Each neutron
detector bank was optimally designed to have seven1-dimensional position-sensitive scintillator detectors,
which are laid vertically. Five 1-dimensional scintillator
detectors have been installed to each bank in the construction phase to reach a horizontal angular coverageof ±15° and an off-angle of 30°. There are ten detectors
in total and four detectors have not yet been installed.
In this year, one detector was installed to the northdetector bank to enhance the neutron detection. The
commissioning and the utilization for the experiments,
together with the installation of another one to thesouth bank will be carried out.
3. Installation of Thermec Master
The Thermec Master’s purpose is to observe theforming process of steel, etc. by in-situ neutron diffraction; it was installed in TAKUMI by the Elements Strategy
Initiative for Structural Materials, Kyoto University andthe BL19 instrumental group. The main specifications
are shown in Table 1. The commissioning was completed
and the utilization started. Using a standard steel sample,
it was confirmed that a 1 sec time-slice analysis was feasible during a forming process at 300 kW beam power.
Table 1. Specification of Thermec Master.
Item
DrivingHeating
Cooling
Maximum temperature
Heating, cooling rate
Working rate
Atmosphere

Specification
Servo motor driving
High frequency heating
Gas injection of N2 or He
1473 K≤ 30 K/s≤ 100 mm/s, 30 kN(compression)
Vacuum or inert gas

4. Development peak profile analysis
One of the advantages of the neutron diffraction
technique compared with other techniques used to determine material characterizations is its high penetrability into materials. Therefore, the neutron diffraction
can evaluate averaged characteristics in bulk samples.
As an advanced analysis technique, the convolutional
multiple whole profile (CMWP) fitting method was introduced into TAKUMI to determine the crystallite size,
the dislocation density, the dislocation arrangement
parameters, and the dislocation character, which isrelated to the fraction of edge and screw dislocations
from line profiles of the whole sample. The demonstration experiment was performed under tensile loading of
as-quenched lath martensitic steel (22SiMn2TiB steel).
5. Development of stroboscopic measurement
The event recording technique was extended not
only for data acquisition of neutron detection, but also
for data acquisition of various conditions of external
fields. By developing a ‘condition filtering data reduction’, we introduced successfully an in-situ stroboscopic
measurement during the cyclic test. This technique wasapplied to a multilayer piezoelectric actuator (PSt150,
Piezomechanik GmbH) to study the behavior of thelattice strain and the domain switching under cyclic
electric field, and revealed that the microscopic deformation estimated from this technique agreed with themacroscopic behavior of the actuator.
6. Development of in-situ neutron diffraction withAE measurement under loading
The acoustic emission (AE) technique is sensitive tointernal motion in the range from several tens of kHz
to several hundred kHz of bulk material. On the other
hand, the neutron diffraction can evaluate the strain
precisely at atomic plane level. Therefore, the combination of the AE measurement and the in-situ neutron
diffraction provide unique information about the deformation mechanism. A development of simultaneous
measurements about the AE and the in-situ neutron diffraction at room temperature has advanced. Then, thistechnique was successfully applied to Mg alloys (AZ31,
Mg85Zn6Y9, etc.).

K. Aizawa1, S. Harjo2, and T. Kawasaki2
Technology Development Section, Materials and Life Science Division J-PARC Center; 2Neutron Science Section, Materials and Life Science
Division, J-PARC Center

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The Current Status of the Versatile Neutron Diffractometer,
iMATERIA
1. Introduction
Ibaraki prefecture, the local government in Japan in
the area where the J-PARC sites are located, has decided to build a versatile neutron diffractometer (IBARAKI
Materials Design Diffractometer, iMATERIA [1]) to promote industrial applications for the neutron beam in
J-PARC. iMATERIA is planned to be a high throughput
diffractometer so that materials engineers and scientists could use it like the chemical analytical instruments in their materials development process.
The roles for neutron diffraction in materials science are (1) to do structural analyses of newly developed materials, (2) to clarify the correlation between
structures and properties (functions), and (3) to clarify
the relation between structural changes and improvements of functions, especially for the practical materials. To achieve those purposes, a diffractometer withsuper high resolution is not required. The matchingamong intermediate resolution around Δd/d = 0.15%,
high intensity and wide d coverage is more necessary.
This diffractometer is designed to look at a decoupled-poisoned liquid hydrogen moderator (36 mm,
off-centered) (BL20), and to have the incident flightpath (L1) of 26.5 m with three wavelength selection
disk-choppers and straight neutron guides with a total length of 14.0 m. The instrumental parameters arelisted in Table 1. There are four detector banks including a low angle and a small angle scattering detectorbank. The angular coverage of each detector bank is

Figure 1. IBARAKI Materials Design Diffractometer, iMATERIA
without detector for each bank and instrument
shielding. The high-resolution bank, special environment bank (90 degree bank), low angle bank,can be seen from right to left. The small angle detector bank, which is not shown in picture, is situated in the low angle vacuum chamber (left handof the picture).

Table 1. Instrumental parameters of iMATERIA. L2 is the scattered flight path. The d-range for each bank is the
maximum value for 2-measurement mode.
L1
26.5m
Guide length
Position of Disk choppers

High
Resolution
Bank
SpecialEnvironment
Bank
Low
Angle
Bank
Small
Angle
Bank

2θ
L2
d-range2θ
L2d-range2θ
L2d-range2q
L2d-range

Total 14m (3section)
7.5m(double)
11.25m(single)
18.75m(single)
150˚ ≤ 2θ ≤ 175
2.0 - 2.3m
0.09 ≤ d(A˚) ≤ 5.0˚
80˚ ≤ 2θ ≤ 100˚
1.5m
0.127 ≤ d(A˚) ≤ 7.2
10˚ ≤ 2θ ≤ 40˚
1.2 - 4.5 m
0.37 ≤ d(A˚) ≤ 58
0.7˚ ≤ 2q ≤ 5˚
4.5 m
1.69 ≤ d(A˚) ≤ 800

also shown in Table 1. The rotation speeds for the diskchoppers are the same with a pulse repetition rate of
25 Hz for the most applications (SF mode). In this case,the diffractometer covers 0.18 < d (Å) < 2.5 with Δd/d
= 0.16% and covers 2.5 < d (Å) < 800 at three detectorbanks of 90 degree, low angle and small angle with
gradually changing resolution. When the speed forthe wavelength selection disk-choppers is reduced to12.5 Hz (DF mode), we can access a wider d-range, 0.18
< d (Å) < 5 with Δd/d = 0.16%, and 5 < d (Å) < 800 with
gradually changing resolution with doubled measurement time from SF mode.
2. Current status
The three banks, high resolution bank (BS bank), special environment bank (90 degree bank) and low angle
bank, are operational and small angle bank is under commissioning. It takes about 5 minutes (DF mode) to obtaina ‘Rietveld-quality’ data in high resolution bank at 500 kW
beam power for about 1 g of standard oxide samples.
Figure 2 is a typical Rietveld refinement pattern
for LiCoO2 sample, cathode material for LIB, at the highresolution (BS) bank by multi-bank analysis functionof Z-Rietveld [2]. It takes 20 min at DF mode to collectRietveld available data, due to high neutron absorption
cross section for natural Li (σsNat = 70 barn).
Small angle detector bank is also start operation
with limited d-range.
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Figure 2. Rietveld refinement pattern for LiCoO2 at high resolution bank of iMATERIA.

3. Sample Environments
The automatic sample changer is the most important sample environment for high throughput experiments. Our automatic sample changer [3] consisted ofsample storage, two lines of elevating system, two setsof pre-vacuum chambers and a sample sorting system.
We can handle more than 600 samples continuously atroom temperature without breaking a vacuum of sample chamber.
The V-furnace (~900 C), the crio-furnace (4 K) andthe 1 K crio are ready for experiment. The gas furnace(~900 C) is under modification.
4. Small sample measurements
Accordingly, the beam power became higher than
before; it is possible to measure the mg samples forabout one day. Small sample measurement is very important for the research for practically materials. We aremaking some trial neutron diffraction measurement forsmall quantities samples. For example, we have measured 25.4 mg YBa2Cu3Oy sample for 18.5 h at 300 kW
beam power. The occupation parameters for deficient
oxygen site are almost same with the result of measurement at 1 g samples. This result supported that theneutron diffraction experiment with mg sample can be
performed.
In small sample measurement, the selection ofsample holder is very important. We have tested LiCoO2
sample using 0.5 mmϕ quartz capillary for XRD. The
sample weight is 7.3 mg for the beam size (2 cm). The
measurement time is only 2 hours and half in 300 kW
due to beam stopped, though 10 hours we expected.
Figure 3 shows Rietveld analysis patterns for this measurement. Measurement time for this experiment isshorter than the time to get enough statistics. But,
Rietveld refinement patterns and obtained parameters
are not so bad. We were planning to longer measurement and measurements for another sample to show
possibility for small sample measurements.

Figure 3. Rietveld refinement pattern for 7.3 mg for beam
size LiCoO2 using quartz capillary at high resolutionbank of iMATERIA.

References[1] T. Ishigaki et al., Nucl. Instr. Meth. Phys. Res. A 600(2009) 189-191.
[2] R. Oishi et al., Nucl. Instr. Meth. Phys. Res. A 600(2009) 94-96.
[3] A. Hoshikawa et al., J. Phys.: Conf. Ser. 251 (2010)
012083.

T. Ishigaki, A. Hoshikwa, Y. Yoshida, T. Matsukawa, and Y. Onuki
Frontier Research Center for Applied Nuclear Sciences, Ibaraki University

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Status of the High Intensity Total Diffractometer(BL21, NOVA)
1. Introduction
Total scattering is a technique to analyze non-crystalline structure in materials. NOVA was designed toperform total scattering and is the most intense powder diffractometer with reasonable resolution (Δd/d ~0.5%) in J-PARC. To realize high statistical accuracy inthe high-Q range, the neutron flight pass between theneutron source and the sample was set at short (15 m)
and the wavelength band width of the incident neutron
was widened (~ 8 Å). It is easy to adapt NOVA to a very
wide field: liquids, glass, local disordered crystalline,
magnetic structure of long lattice constant and so on.
The observation of the hydrogen position in materials
is one of the most important scientific themes of NOVA.
2. Sample environment
For effective measurements with intense neutron
flux at the 1-MW operation, a faster and automatic sample exchange is important. A temperature-controlled
auto sample exchanger (Fig. 1) was fabricated to realize
such an experiment. It can load 12 samples and users
can perform the experiment sequentially as an automatic measurement: timing of the exchange of sample
on neutron beam and the sample temperature (10 K ~500 K). A top loading cryostat was also introduced forthe measurement in the temperature range between
5 K ~ 700 K. An automatic sample exchanger with40 samples for room temperature measurements will
be ready in FY 2015.

3. Data reduction software
The goal of the data reduction of total scattering is
to obtain static structure factor, S(Q),S(Q) =(1)

where, b is scattering length, σcoh is coherent crosssection, Ω is solid angle, respectively. It is essential
for total scattering to obtain an absolute coherent
cross section from the observed intensity by the data
reduction. Since pair correlation functions will be obtained from S(Q) by Fourier transform, the reliability of pair correlation functions simply relies on thereliability of S(Q).
However, it is not always trivial to get the absolutevalue and the users need to check whether the reduction is satisfactory. To help with this, the reduction
software of NOVA outputs intermediate data as crosssection value. Figure 2 shows typical outputs from the

(a)

(b)

(c)

Figure 1. Temperature controlled auto sample exchanger ofNOVA.

1 ⎛ dσcoh− <b2> + <b2>⎞⎠<b2> ⎝ dΩ

S(Q) =

1 ⎛ dσcoh− <b2> + <b>2⎞⎠<b2> ⎝ dΩ

Figure 2. Typical three snap shots of the data reduction process of SiO2 glass on NOVA. (a) multiple scatteringand incoherent cross section, (b) obtained coherent cross section (blue) and (c) calculated cross section with table value and bottom: S(Q) converted
from coherent cross section with equation (1).

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data reduction software of NOVA. Input parameters ofsample information such as bulk density (no. of sample
atoms in a beam) and concentration will be checked.
If necessary, further corrections with inverse Fouriertransform, fitting with polynomial function and selfterm correction with Powles method [1] and null-H2O
method [2] will be performed.

References[1] J. G. Powles, “The analysis of a time-of-flight neutron diffractometer for amorphous materials: thestructure of a molecule in a liquid”, Mol. Phys. 26,
1325 (1973).
[2] Y. Kameda et al., “Inelasticity Effect on Neutron
Scattering Intensities of the Null-H2O”, Journal of
Neutron Research, 11, 153 - 163 (2003).

T. Otomo1, K. Ikeda1, H. Ohshita1, N. Kaneko1, T. Seya1, and K. Suzuya2
Institute of Materials Structure Science, KEK; 2Materials and Life Science Division, J-PARC Center

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Current Status of the Energy-Resolved Neutron Imaging
System “RADEN”
1. Introduction
The Energy-Resolved Neutron Imaging System,
RADEN, installed at beam line BL22 in MLF, is the first
instrument in the world dedicated to pulsed neutron
imaging [1]. The aim of this instrument is to carry out
not only energy-resolved neutron imaging experiments
but also state-of-the-art neutron radiography and tomography experiments using the pulsed neutron
beam. The construction of RADEN started in 2013 andthe neutron beam was transported for the first time in
November 2014 (Fig. 1). After the first beam, we began
on-beam commissioning of RADEN to clarify its performance and perform some demonstration experiments.
2. Commissioning of RADEN
To confirm the performance of RADEN, commissioning studies have been carried out. There were several items that had to be characterized. In terms of thebasic neutron beam characteristics, the spectrum, thepulse width and the beam intensity were investigated.
Also, for the image acquisition, the available field ofviews and L/D ratios were confirmed by changing theaperture sizes and positions and compared with the expectations. As a result, a maximum FOV of up to 300 ×
300 mm2 was achieved. To characterize the optical device performance, the T0 chopper and the double-disk
low-speed chopper were tested. Using the T0 chopper,
while the accessible shortest neutron wavelength was
restricted to 0.43 Å, the high energy neutron intensity
and the prompt burst were decreased to about 10−4 ofthat without the T0 chopper. The double-disk chopper,used to define the wavelength range by changing the
opening angle of two disks, was confirmed to provide
the neutron beam with well-defined wavelength range
and remove properly the higher frame. Moreover, setting
one disk in counter-rotation direction and at the smallest opening angle, we can obtain monochromatic beamwith coarse wavelength resolution of about 10% bychanging the phase of the rotating disks (Fig. 2). Hence,these choppers enable us to conduct neutron radiography experiments with a white or a monochromatic beam
easily by just changing the condition of the choppers. As
the polarized neutron imaging is planned in RADEN, theneutron polarization devices are installed in the beam

Figure 1. Left: Photograph taken at the time of the first beam. Center and right: first radiographs.

Figure 2. On-beam commissioning results. Left: neutron spectrum (red marker: experiment, blue line: simulation). Right: results ofthe double disk chopper test to obtain monochromatic beam with coarse wavelength resolution.

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MLF Annual Report 2014line as optional equipment. The polarizability of the device was studied, and the maximum polarization was
confirmed to be 97% at a wavelength longer than 5 Åand the critical wavelength was found to be 1.5 Å. Thoseagreed well with the designed values. However, because
small polarization oscillation against the neutron wavelength was observed, improvement in the magnetic field
connection is necessary.
Several two-dimensional neutron detectors are prepared in RADEN. For the conventional neutron radiography and tomography, CCD-based camera systems areused, while to perform energy-resolved neutron imaging, which requires accurate measurements of neutronenergy by means of time-of-flight technique, counting type neutron detectors, the μNID [2], the nGEM [3],and a pixelated Li-glass scintillator detector [4], areused. The fundamental performance of detectors, suchas spatial resolution, linearity, counting rate, and efficiency, was studied in the commissioning. Fig. 3 shows
typical result of a spatial resolution measurement using
standard indicators. Using CCD-based detector, a spatial resolution of around 300 μm was reached, with the
FOV of 300 mm and around 100 μm with selected FOV
using a neutron image-intensifier system. We continue
the improvement of the detector system to increase thehomogeneity of the scintillator screen and obtain muchfiner spatial resolution.

Figure 3. Image of the standard indicator. Left: overall imageof the indicator (PSI Siemens star), right: enlarged
image. Gaps with 100 μm width are visible.

3. Demonstration experiments
In addition to the commissioning, we have performed some demonstration experiments of the conventional neutron imaging and the energy-resolved
neutron imaging, i.e., Bragg-edge, resonance absorption, and polarized neutron imaging. In RADEN, neutron CT experiments can be performed automaticallyby computer-controlled motorized sample stage and
CCD camera system. Fig. 4 is an example of a CT reconstructed image of bearings. This is the first result of CT
experiments using the pulsed neutron beam.

Figure 4. Example of a CT reconstruction image of bearings.

4. Summary
We have completed the construction of the energy-resolved neutron imaging system, RADEN, and began the commissioning study with the pulsed neutron
beam. Together with the performance confirmation experiments, we conducted some demonstration experiments in both the conventional neutron radiography/
tomography and the energy-resolved neutron imaging.
We plan to start the user program from FY 2015.
References[1] T. Shinohara, T. Kai, Neutron News, 26 11 (2015).
[2] J. D. Parker et al., Nuclear Inst. and Meth. Phys. Res.,
A726 155 (2013).
[3] S. Uno et al., Phys. Proc. 37 600 (2012).
[4] S. Satoh, JPSJ Conf. Proc. 8 051001 (2015).

T. Shinohara1, T. Kai1, K. Oikawa1, T. Nakatani1, M. Segawa1, K. Hiroi1, Y. Su1, H. Hayashida2, J. D. Parker2, Y. Matsumoto2, S. Zhang2,
and Y. Kiyanagi3
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center, JAEA; 2Neutron R&D Division CROSS-Tokai; 3Nagoya
University

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BL23 Polarized Neutron Scattering Spectrometer POLANO
1. Introduction
The success of the chopper spectrometer MARI applied to materials science at the ISIS neutron facility has
highlighted the importance of the so-called chopper
spectrometers to neutron beam line instruments. At theJapan Proton Accelerator Research Complex (J-PARC),
the Materials and Life Science Experimental Facility(MLF) is a newly constructed world-leading pulse neutron experimental facility, where three chopper-type
spectrometers are now part of the research program.
One of the remaining technical issues that should beapplied at MLF is the use of a polarization neutron technique with a pulsed neutron beam. Although the polarized neutron technique has been developed and used
for many years, the application of the time-of-flight(TOF) method has been put into practice only in the
recent years. In particular, with regard to the inelastic
spectrometer, the polarized neutron technique finds
limited practical use in wide scattering angle instruments. The use of the polarized neutron technique option has been planned for some of the elastic neutron
instruments, such as a small angle scattering instrument, a reflectometer, a single crystal diffractometerand an imaging instrument, but not yet for the instruments dedicated to the inelastic scattering. In the lightof recent discoveries in material science, many of theobserved complex phenomena are predominantly due
to the entangled physical degrees of freedom of spins,
charges, orbitals, and even lattice vibration. In neutron
scattering experiments, the varying dependence of
momentum, energy, and temperature can be interpreted by these degrees of freedoms. However, a unique,effective, and direct way to observe these properties
separately is via polarization analysis. Thus, the polarized neutron experiments are quite significant for material science particularly for research on magnetism,hydrogen materials, and strongly correlated electron
systems with multiple physical degrees of freedom.
2. Construction of the spectrometer
The project was launched in 2009 starting as an
S-type project with financial support from the KENS
neutron facility. After the budget for the project was
successfully sanctioned and obtained, the actual construction began in 2013. In 2014, many of the main
beam line components have been designed, manufactured, tested and installed [1-3].
A vacuum chamber (VC) is one of the crucialcomponents, where neutron detectors are positioned
at its end. The dimensions of the chamber are approximately 4 × 3 × 3 m and its weight is 20,000 kg, as depicted in Fig. 1. This type of large VC is normaly made ofsteel, whereas stainless steel was used for POLANO VC
to avoid magnetic interactions. Neutron detectors (position sensitive detectors (PSD)) are installed at the endof the chamber (called “detector banks”). The detectorbanks were designed to make the install and change
of PSDs easy by opening and closing the bank hanging
on the trolley. Inside the VC, a B4C liner was fixed on thewall as a neutron absorber eliminating the unintended
scattering from the wall and other materials inside.

Figure 1. Newly installed large vacuum chamber.

Epoch-making in the design of the VC was the creation of one large chamber composed of three parts(sample chamber, scattering chamber and a part inbetween the two (we call it “joint chamber”)). Since
the sample chamber and the scattering chambers canbe evacuated separately, the joint chamber can be removed and put some devices in the position as spin
flipper. Another remarkable feature is that in the scattering chamber a large trestle table for analyzer mirror
has been set into the VC. The table can rotate in vacuum
and even its rotational and tilting angles can be finetuned. As the analyzer mirror mounted on the table will
weigh 80 kg, the frames of the trestle need to be robust
and able to be accurately controlled in vacuum. A moving test has been performed in a factory as shown in
Fig. 2, then the device was installed at the MLF beamline with the VC.
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Figure 3. Newly assembled POLANO Fermi chopper rotor (a)and the display of the chopper rotational speed at
the spinning test (b).

Figure 2. The trestle and moving system for analyzer mirror,
testing at a factory with 80 kg dummy load.

After many designing reviews other devices were
included in the manufacturing schedule. Choppers aresome of the beam-line components, which are utilized
for shaping the neutron pulse, eliminating the background, and monochromatizing the neutron energy.
Four different types of choppers are used in POLANO,
namely T0 chopper, disk choppers (25 Hz), Fermi chopper and fast rotating disk chopper. Fig. 3 depicts the
newly designed Fermi chopper for POLANO. In the spinning test, the payload was nicely controlled and 600 Hzof the rotor rotation was achieved. The required phaseaccuracy at 600 Hz was 0.3 μs, the acquired phase accuracy 0.18 μs was satisfactorily achieved.

This year neutron guide tubes with 4 Qc super mirror are ready to be installed in the beam line. The use ofan elliptical guide tube provides a flux that is 10 times
higher than in a no-mirror guide tube (collimator) evenfor 100 meV neutrons. For the monochromatic beam,
we also evaluated the neutron flux at the sample position and the resolution of the diffracted beam at thedetector position by using McStas [4, 5]. Since POLANO
is aimed at the incident neutron energy range up to Ei =100 meV, the evaluated intensity and resolution below
100 meV were found reasonable for conducting polarization analysis experiments.
References[1] T. Yokoo et al., J. Phys. Conf. Series 502, 012045(2014).
[2] T. Yokoo et al., J. Phys. Soc. Jpn. 82, SA035 (2013).
[3] K. Ohoyama et al., J. Phys. Conf. Series 502, 012051(2014).
[4] K. Lefmann and K. Nielsen, Neutron News 10, 20(1999).
[5] P. Willendrup, E. Farhi and K. Lefmann, Physica B
350, 735 (2004).

T. Yokoo1,2, K. Ohoyama3, S. Itoh1,2, M. Fujita3, N. Kaneko1,2, S. Sugai1,2, M. Ohkawara3, T. Ino1,2, and M. Sakaguchi1,2
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3Institute forMaterials Research, Tohoku University

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Status of the Common Technical Development
1. Overview
To achieve the 1-MW operation on neutron instruments in MLF, the common technical issues are selected
and the work on their development is performed by individual teams which include JAEA, KEK and CROSS staffs.
The selected common technical issues are the realization of the polarized-neutron scattering technique,the utilization of a common sample environment, theestablishment of advanced computational environment, and the fabrication of high performance neutron
choppers. Specifically, these works have been carriedout by the 3He SEOP team, the sample environment
team, the computational environment team and the
chopper team, respectively.

phase 1, the users can login in the MLF computational
environment, including individual BL computers, andobserve the status of the experiment. The development of phase 1 was completed in JFY 2014 and several BLs started to use the remote access function. As anext step, phase 2 and phase 3 are planned. Users canperform advanced analysis by virtual environment atphase 2. Further analysis environment combined withvarious simulation tools will be provided in phase 3.
In JFY 2014 the MLF experimental database was redesigned to treat large data effectively. The main areasof development were data access function, web portal function, database link function and access control
function and these functions were added successfully.

(1) 3He SEOP team
A prototype of an in-situ SEOP 3He spin filter as ananalyzer for BL17 was constructed, and good polarization performance was observed at the beam line. Also,a demonstrative SANS study of hydrogen-containedmaterial was performed at the BL15, and the coherent
and incoherent scattering components were successfully extracted by the polarization analysis by using an
off-line SEOP 3He spin filter.

(4) Copper team
It is very important to fabricate highly reliable
choppers, especially a T0 chopper, because their components, such as the hammer of the T0 chopper, will behighly activated due to the high dose at a 1-MW operation. Therefore, the requirements for new T0-chopper’s
performance include an expanded maintenance period, which should be as long as possible with a very low
failure probability. The design of a new highly reliable
T0-chopper was completed while taking into accountthe operational experience of the current machine. Its
rotational speed specification is 100 Hz. Figure 1 shows
the drawing of new T0 chopper. Its dimensions are
820 mm wide, 494 mm long, and 860 mm high. The designed maintenance period is 39,200 hours.
The assembling, operational test and evaluation of
the test equipment will be performed the next year.

(2) Sample environment teamCommissioning and improvements were performed by the sample environment team on thevertical-field superconducting magnet, the high temperature furnace and the 3He cryostat, which are standard common sample-environments in MLF, while thedevices were operating. The development of a pulsed
magnet system for neutron diffraction, which is defined
as an advanced sample environment in MLF, was carriedout. The high-voltage unit for 30 T class high-magnetic
field was assembled in JFY 2014. Test neutron scatteringexperiments will be performed the next year.
(3) Computational environment team
One of the user requests about computational environment is for a remote access to the MLF computational environment, including individual BL computers.
Phase 1 is defined as a first stage in the development of
the advanced computational environment in MLF. At

Figure 1. Drawing of the new high-performance T0- chopper. Its maximum rotational speed is 100 Hz.

K. Aizawa and T. Oku
Technology Development Section, Materials and Life Science Division, J-PARC Center

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Development of an in-situ SEOP 3He Neutron Spin Filter
1. Introduction
We have been developing an in-situ spin-exchange
optical-pumping based polarized 3He neutron spin filter(in-situ SEOP 3He NSF) for efficient utilization of pulsed
neutrons at J-PARC. In this study, i) we have developed
a prototype of the in-situ SEOP 3He NSF as the analyazer for the polarized neutron reflectometer SHARAKU(BL17) and evaluated its performance at the beamline,ii) we have developed the in-situ SEOP 3He NSF as thepolarizer for the polarization analysis neutron spectrometer POLANO which is under construction.
2. The in-situ SEOP 3He NSF as the analyzer for thepolarized neutron reflectometer SHARAKU (BL17)
Figure 1 shows the constructed 3He NSF as a prototype for SHARAKU. All of its components were put in a laser shield box made of black anodized aluminum boards
for laser safety. The dimensions of the laser shield box are
605 mm × 605 mm × 350 mm. The 3He cell was installed
in a solenoid coil with a double layered Permalloy magnetic shield. The size of the 3He spin filter cell was 35 mm
in diameter and 55 mm in length. The 3He-gas pressure
length product of the cell was 11 bar-cm. The magnetic
shield was designed for the in-situ 3He NSF with a cell sizeof 100 mm in diameter and 100 mm in length under aperipheral magnetic field of several tens Gauss.
We set up the 3He NSF in a scattering chamber of
SHARAKU and evaluated its performance in terms ofthe maximum 3He polarization, the relaxation time
constant of the 3He polarization and the magnetic
guide field for polarized neutron beam transportation.
Figure 2 shows a schematic layout of the experimental
setup at SHARAKU. We used a magnetic supermirror topolarize the incident neutron beam and a Drabkin spin
flipper to change the polarization of the neutron beam.
Those devices were installed in the shield upstream ofthe sample position. A guide field was applied along

Figure 1. The prototype of the in-situ SEOP 3He NSF for
SHARAKU.

the neutron beam path to transfer neutrons while conserving the neutron spin state. The 3He NSF was placedin the scattering chamber. The reflected neutrons wereanalyzed by using the 3He NSF and 3He detector (Fig. 2).
We checked the magnetic guide field of SHARAKU forpolarized neutron beam transportation (Fig. 2). Two solenoid coils were placed at the upstream of the sample
stage and inside the scattering chamber. The strengthof solenoid coil’s magnetic field was >10 G, strong
enough to keep the polarization of the neutron beam.
The direction of solenoid coil’s magnetic guide field wasparallel to the neutron beam axis (z-axis) (Fig. 2). We applied a magnetic field of 20 G onto the 3He cell along
the neutron beam axis.
After the adjustment of the magnetic guide field,
we started the optical pumping of the 3He gas to polarize it. The time development of the 3He polarization wasmonitored by using the AFP-NMR, as shown in Fig. 3.
Here, the amplitude of the AFP-NMR signal is proportional to the 3He polarization degree. Thus, we can estimate the 3He polarization from the AFP-NMR signal byusing the conversion parameter.

Figure 2. Schematic layout of the experimental setup at SHARAKU.

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Finally, we evaluated the 3He polarization by using
unpolarized neutrons. We measured the intensities of
the neutrons transmitted through the 3He NSF in polarized and unpolarized 3He gas conditions. The obtained
neutron intensities are shown in Fig. 4 (a). The 3He polarization degree was calculated to be 56.9% based on
the neutron transmission measurements (Fig. 4 (b)). The
result was well consistent with the value determined by
the AFP-NMR.

Figure 3. The time development of the 3He polarization measured by the AFP-NMR.

The laser power supply for the optical pumping
was stopped several times due to a temperature error
with the laser diode. The SEOP box had a cooling fan
to keep the temperature low inside the box. However,since the temperature within the scattering chamber,in which the SEOP box was located, rose with time, atemperature error occurred. We added the fan to lower
the temperature of the scattering chamber. However,the system was stopped several times even after the improvement. So we had to reduce the laser power down
to the moderated level to ensure a stable operation.
The maximum 3He polarization P3He was determined
to be 56.9% by the AFP-NMR (Fig. 3). By analyzing thetime development of the 3He polarization during theoptical pumping, it was estimated that the maximum
3He polarization P
3He reached about 62% (Fig. 3). The relaxation property of the 3He polarization was measured
after the laser irradiation and the heater were stopped.
The relaxation time constant was 75 hours.

3. The in-situ SEOP 3He NSF as the polarizer forthe polarization analysis neutron spectrometer
POLANO (BL23)
We have been developing a compact system of
the in-situ SEOP 3He NSF for the limited space of the
POLANO. A schematic view of the 3He NSF in POLANO
is shown in Fig. 5.
We will prepare cylindrical cells made of GE180 aluminosilicate glass with diameter of 60 mm and lengthof 60 to 100 mm. The cells will be filled with 3He at 2.0
to 3.5 atm, and the effective 3He thickness would range
from 12 to 35 atm-cm for various measurements.
A solenoid and compensation coils at both solenoid edges with Permalloy magnetic shield were designed, and a proto-type magnet has been constructed.
The neutrons are polarized in the axial direction in the
3
He NSF, and the spins are rotated adiabatically in thetransverse direction by the magnetic guide field. The
compensation coils will be optimized according to theguide field.
A laser diode array with an output power of 100 W
with a chirped volume Bragg (holographic) grating(VBG or VHG) emits a spectrally narrowed 795 nm (RbD1 line) for the optical pumping of Rb (Fig. 6). A quarter(a)(b)
Figure 4. (a) Intensities of the neutrons transmitted through the 3He cell with the polarized and depolarized 3He, and (b) 3He polarization determined by the neutron transmission measurements.

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Figure 5. A schematic view of the 3He NSF in POLANO. Allessential elements are packed in a laser shield box
with a size of 600 mm × 600 mm × 250 mm.

waveplate converts linear polarization into circular polarization. The waveplate can be remotely rotated by+/−90 degrees to change the left and right states according to the AFP spin flipping of 3He. The laser optical
apparatus is shown in Fig. 7.
In SEOP, hot air blowers (compressed air blowers)
are commonly used to keep 3He cells at an elevatedtemperature because they do not interfere with the homogeneous magnetic field while conventional electricheaters produce unnecessary magnetic fields. However,a hot air blower occupies a fair amount of space andrequires heat insulation around itself for safety. Dueto the limited available space, we have decided not to
use a hot air blower but a thin electric heater made ofpolyimide films and NiCr strips, which is attached to theouter surface of an aluminum oven for a 3He cell. The
NiCr strips will be designed specifically to minimize themagnetic field interference.
In almost all measurements with polarized neutrons, neutron spin flipping is a must for cancellingout any systematic uncertainties. We have successfully
demonstrated a compact AFP spin flipper for polarized 3He with an RF coil positioned inside an aluminumoven. The 3He spins can be flipped within half a second,
and the polarization loss was measured to be less thanFigure 6. Laser spectra from the 100 W laser diode array(LDA) with and without the chirped volume Bragg
grating (C-VBG). Not only is the spectrum narrowed
but also the peak intensity is much higher with theuse of the C-VBG.

4 × 10−4 in one spin flip. Such an AFP spin flipper will beredesigned to fit the 3He cells described previously.
4. Conclusion
In conclusion, we are developing the in-situ SEOPNSF as the analyzer for SHARAKU and POLANO. The
main components have been almost developed, andwe are going to fix some problems and/or optimize theoperation parameters for application at the beamlines.

Figure 7. A picture showing the laser optical apparatus, a laser diode array (LDA), a chirped volume Bragg grating (C-VBG), and a quarter waveplate.

T. Oku1, T. Ino2, K. Sakai1,3, K. Hiroi4, T. Shinohara4, K. Aizawa1, M. Arai5, M. Takeda6, K. Kakurai6, H. Kira7, H. Hayashida7, N. Miyata7,
K. Akutsu7, J. Suzuki7, M. Ohkawara8, and K. Ohyama8
1
Technology Development Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science,
KEK; 3Neutron Source Section, Materials and Life Science Division, J-PARC Center; 4Neutron Science Section, Materials and Life Science
Division, J-PARC Center; 5Materials and Life Science Division, J-PARC Center; 6Quantum Beam Science Directorate, JAEA; 7CROSS-Tokai;
8Institute for Material Research, Tohoku University

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Sample Environment at MLF
1. Introduction
The SE team is working on adopting and operating the so-called beamline (BL)-common SE equipment, and on developing new SE equipment. We
currently have a vertical-field superconducting magnet,a 3He-4He dilution refrigerator insert and a high-temperature furnace as the BL-common SE equipment. In
JFY2014, three new members (JAEA: 1, CROSS: 2) werejoined the SE team, and then a total of 13 members
were divided into sub-teams, such as cryogenics andmagnets, high temperature, high pressure, soft-matter,and development. The development items are a pulsed
magnet system, a low-temperature and high-pressure
environment equipment and a hydrogen environment
equipment.
2. Operation of the BL-common SE equipment
In April, 2014, we operated the superconducting
magnet at BL17 for its commissioning of polarized neutron reflectivity measurement. The applied magnetic
field was from 1.00 T to 6.00 T at a base temperatureof 4.2 K during the operation. Following the operation
at BL17, we have performed the commissioning at the
SE area, and then VTI (Variable Temperature Insert)
reached 1.068 K, the lowest temperature ever registered by a single shot mode. In this period, three CROSS
members in the SE team joined the operation from the
setup of the superconducting magnet at the SE area
(Fig. 1) for the first time since the current SE team wasorganized.

Figure 1. Setup of the 7T superconducting magnet at the SE
area (liquid He transfer).

Along with our task of supporting the users of theexperiment, we also work on improving the BL common
SE equipment to make it easier to use. We modified ahigh temperature furnace with niobium heater to improve the convenience and safety in users experiment.
In the last fiscal year, we installed a control panel for thevacuum pumping system and an electric distribution
board, as well as equipped an argon gas inlet line forexperiments under argon atmosphere. To make further
improvements, we equipped the system with automatic vacuum evacuation and argon gas inlet (Fig. 2).
In addition, we introduced a touch panel device, which
made it possible to integrate various pieces of information, such as the settings parameters and an alarm listof all controllers, heating conditions and so on.

Figure 2. Improved vacuum pumping system of a high temperature furnace.

3. New equipment and development
In JFY2014, a new closed-cycle 3He cryostat was
introduced as part of the BL-common SE equipment.
This cryostat is a one-shot 3He system including a pulse
tube refrigerator to precool 3He. Its lowest temperature
is 0.3 K, which can be maintained about 50 hours without sample. The system is automatically cooled down
to the lowest temperature within 24 hours. The cryostat
was designed to fit the goniometer. A rotation stage to
fit it to the vacuum chamber will be fabricated in thenext fiscal year.
With the magnet technologies we can perform diffraction experiments, small angle scattering, inelastic
scattering and so on. Recently, measurements using
neutron beams have been rapidly developed underhigh magnetic field. We developed a prototype of compact power supply in J-PARC MLF. Figure 3 shows theappearance of the power supply. The size is as follows:
760 mm in width, 1000 mm in depth, and 1400 mm
in height. Maximum charged voltage and output current is 2 kV and 8 kA respectively. Repetition rate is one
119Neutron Science

MLF Annual Report 2014

pulse every several minutes. The pulse duration is a few
milliseconds.
The operation examination of the power supply
was performed using a solenoid coil (200 μH) as a load.
The obtained peak current was approximately 7.7 kA
when the charged voltage of the capacitor was 2 kV.
A new coil and a sample stick is being developed
for the neutron scattering experiment.

760
m

10
00
m
m

1410mmFigure 3. Photograph of the power supply.

The SE high-pressure sub-team started their substantial activities in JFY 2014. In the MLF, there is abeamline dedicated for high-pressure experiments(BL11). Furthermore, some groups have carried out
their experiments under high-pressure with their own
high-pressure apparatus. However, so far we did nothave a high-pressure environment device as part of theBL-common equipment. Therefore, we held an opinionexchange meeting with each BL staff in charge, anddiscussed the development of high-pressure environments. In JFY 2014, VX-6 type Paris-Edinburgh press(with capacity of 130 tons), widely used in neutron
facilities, was introduced as the first BL-common highpressure device. Expansion into low-temperature environment is also planned.
4. SE Workshop
The 8th International Workshop on Sample
Environment at Neutron Scattering Facilities was heldin Oxford, UK, October 12-16 2014. It included 70 participants from 16 facilities in 11 countries, including
4 members from J-PARC/MLF. T. Aso reported on thecurrent status of SE at MLF, Y. Yamauchi introduced
the activities in managing the SE equipment at MLF,
and K. Munakata presented the development of highpressure sample environment for single crystal neutron diffractometer SENJU at J-PARC MLF. During theworkshop, there was a meeting of ISSE (International
Society for SE), an organization for activate collaborations and information sharing among the facilities, S.
Ohira-Kawamura attended the meeting. At the event it
was decided that the next SE workshop will take placeat near NIST, USA, in 2016.

Figure 4. Photograph of workshop members at EynshamHall, Oxford, UK.

T. Aso1, Y. Yamauchi2, M. Ishikado3, S. Ohira-Kawamura4, M. Watanabe2, K. Munakata3, S. Takata4, Y. Sakaguchi3, K. Ohuchi3,
M. Obinata3, T. Yokoo4,5, W. Kambara2, and R. Takahashi61
Neutron Source Section, Materials and Life Science Division, J-PARC Center; 2Technology Development Section, Materials and Life Science
Division; 3Neutron R&D Division CROSS-Tokai; 4Neutron Science Section, Materials and Life Science Division, J-PARC Center; 5Institute ofMaterials Structure Science, KEK; 6Nippon Advanced Technology co.

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Present Status of the MLF Experimental Database
1. Introduction
The neutron instruments in MLF create a hugeamount of experimental data. A typical volume of data
produced in one experiment is from several tens MB
to several hundreds GB. Since a lot of experiments under various experimental conditions are carried out ina short period of time using high-intensity beams, thetotal amount of data generated annually in a whole facility at full performance is in the order of PB. In thosesituations, it is required to safely and efficiently manage
a huge amount of data over a long period of time. In
particular, an appropriate protection and preservationof the experimental data produced at MLF as intellectual property is required. Furthermore, it is needed toprovide the facility users with a data access service enabling the effective utilization of a lot of experimental
data.
To meet these requirements, we are developing
and operating the MLF experimental database (MLF
EXP-DB) shown in Fig. 1. The main features of the MLF
EXP-DB are as follows: [1] Data Management
 Experimental data cataloging (online/offline) Centralized raw data management (registration, archive, retrieve)
 Data Access Browsing/Searching the meta-data catalog
 Downloading raw data and meta-data Executing simple data analysis
 Web portal
 Web-based interface for data management
and access Database Link
 Collecting user, proposal and sample information from other databases
 Access Control
 Authentication and Authorization
2. Recent update features
Recently, we have redesigned the MLF EXP-DB toenhance the availability and scalability, and improveda function of the experimental data retrieval in the web
portal.
For the core system of the data management infrastructure, high availability is required. A service
outage caused by system failure and maintenance applying patches should be avoided as much as possible.
A redundancy of the system allows avoidance of suchservice outage, so that the availability is improved. We
have turned the system into a redundant distributed
system.
It is also necessary to consider scalability of the system especially in data cataloging. The data production
rate in the facility is continuously rising. It depends on
the beam intensity and the performance of the neutron
instruments. In MLF, the beam intensity has been increasing in phases according to the development planfor the accelerators and the neutron sources. The scaleof the experimental data catalog will be in the order oftens of millions of tags recorded in XML-format at fullpower operation in MLF. Also, the additional installation of detectors and improvement of various devices
in the instruments have been increasing consistently.
Considering this situation, we have improved the MLF
EXP-DB into the system to be capable of scaling-out responding to the scale of data quantity produced in thefacility.
Furthermore, an improvement of the experimental
data retrieval can promote better data utilization. We
have improved the experimental meta-data retrieval
with a flexible search settings according to the experimental conditions.
High Availability
The improved redundant system is composed oftwo servers in a switch over relationship. When one ofthem is operated as an active server responsible for collecting experimental data from the instrument’s local
systems and data access, the other is operated as a hotstandby server. The database replication is regularly
performed from the active server to the hot-standby
server. In the case of system failure or maintenance, theactive server is switched. The data access is provided
via a front-end web server, so that the users need not totake account of the access destinations.
Scaling-out
The system has been scaled out to improve scalability for the data cataloging. It is composed of thetwo redundant system units mentioned in the previous
subsection. There are two experimental halls in MLF.
Currently, one system is allocated to the instruments in
the 1st experimental hall and the other system is allocated to the instruments in the 2nd experimental hall.
It is capable of performing further scaling out of a load
distribution by adding the redundant systems responding to the data production rate.

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MLF Annual Report 2014ᵳᶑᶃᶐᶑᴾᶍᶄᶄᶇᶁᶃᵆᵳᵭᵇ
ᵢᵿᶒᵿᴾᵟᶁᶁᶃᶑᶑ

ᵫᵪᵤᴾᵣᵶᵮᵋᵢᵠᵢᵠᴾᵪᶇᶌᶉᵌ
ᵆᵮᶐᶍᶎᶍᶑᵿᶊᵊᴾᵳᶑᶃᶐᵊᴾᵱᵿᶋᶎᶊᶃᴾᵧᶌᶄᶍᵌᵇ

ᵢᵿᶒᵿᴾᵮᶐᶍᶁᶃᶑᶑᶇᶌᶅ
ᵰᵡᵫᵱᶗᶑᶒᶃᶋ
ᵱᵱᶍᶄᶒᶕᵿᶐᶃ
ᵡᶍᶋᶎᶓᶒᶇᶌᶅᴾᵰᶃᶑᶍᶓᶐᶁᶃ

ᵟᶐᶁᶆᶇᶔᶃ
ᵣᶖᶎᶃᶐᶇᶋᶃᶌᶒᵿᶊᴾᶂᵿᶒᵿᵮᶐᶍᶎᶍᶑᵿᶊᴾᵢᵠᵡᶍᶋᶋᶍᶌᴾᵢᵿᶒᵿᴾ
ᵱᶒᶍᶐᵿᶅᶃ

ᵰᵿᶕᴾᶂᵿᶒᵿᴾᵿᶌᶂᴾᶋᶃᶒᵿᵋᶂᵿᶒᵿ

Figure 1. The schematic view of the MLF experimental database (MLF EXP-DB).

Flexible Data Retrieval
Since various sample environmental apparatusesin neutron instruments are used depending on the purpose of the experiment, the structure of the experimental meta-data can be changed with every experimentor instrument. Although every variety of information
associated with the experimental conditions as experimental meta-data in XML-format is registered in the experimental data catalog, in the conventional retrieval
function the options are limited to some basic information on the experiment such as run No., date and time,
experimental title, and primary investigator. In the improved retrieval, it is possible to execute a flexible data
search for more information by specifying the search
conditions for each tag of experimental meta-data corresponding to the device condition.
3. Conclusion and future plans
We are operating and updating the data management infrastructure in J-PARC/MLF. The infrastructure ismainly composed of the MLF EXP-DB, which is responsible for data management and access, and the datarepository for the central preservation of experimental raw data and meta-data. Currently, it manages theexperimental data at four neutron instruments (DNA,PLANET, SHARAKU and SENJU) in MLF and it is planned
to expand the management to other instruments soon.
The MLF EXP-DB provides the web portal as the interface for data management and access. The web portal
offering data access for facility users is under trial use.
We will start the data access service with this web portal, including the flexible data retrieval, next year.
We have also improved the MLF EXP-DB by redesigning the redundant and scaling-out system. We havea plan for a performance evaluation in the near future.
Reference[1] T. Nakatani, Y. Inamura, K. Moriyama, T. Ito, S. Muto,
T. Otomo, “Event recording data acquisition systemand experiment data management system for neutron experiments at MLF, J-PARC” JPS Conference
Proceedings Volume 1, 014010, 2014 (Proceedingsof the 12th Asia Pacific Physics Conference).

K. Moriyama and T. Nakatani
Technology Development Section, Materials and Life Science Division, J-PARC Center122

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Supermirror Coating for Special Figuring
1. Large-m supermirror coated on thin silicon
substrate
For supermirror benders and polarizers, thinnersilicon substrate is adequate to provide better transmission efficiency, because substrate materials have serious effect on the total cross-section.
We fabricated NiC/Ti supermirrors (m = 5) coated on
Si substrates with 0.1 mm thickness. A total of 5,000 layers was coated on the both sides of the Si substrates.
An ion beam sputtering instrument [1] with a coatingarea of 50 cm in diameter was used. Figure 1 shows asubstrate holder on which 74 substrates with size 20 ×
50 mm were set in the large-scale instrument.

We have been developing a Wolter type I supermirror, which consists of ellipsoid-hyperboloid of revolution. In order to fabricate the Wolter mirror, replica
method is applied and NiC/Ti supermirror was coatedon a mold with aspherical shape [3]. Figure 2 shows amold holder which has spin rotating mechanism forcoating around the mold and the whole substrate holder which rotates for spatially-homogeneous coating in
the ion beam sputtering instrument.

b) rotation for spatially-homogeneous coatinga)rotation for coating around the mold

50 cm

Figure 1. The substrate holder with 74 substrates of the ion
beam sputtering instrument.

The neutron reflectivity of the m = 5 supermirror
was 70% at the critical angle, and the profile gradually
increased to the total reflection.
2. Supermirror coating on aspheric-cylinder
substrate
The neutron focusing mirrors play an importantrole to enhance the neutron intensity at a sample position or to improve the q-resolution of small angle scattering experiments. For 3-dimensional focusing optics,
Kirkpatrick-Baez (K-B) mirrors were developed for having intense neutron beam by using elliptic supermirrors(m = 4) [2].

Figure 2. The substrate holder on the ion beam sputtering
instrument; a) the mold holder which has spinrotating mechanism and b) the whole substrateholder which has rotating mechanism for spatiallyhomogeneous coating.

The NiC/Ti supermirror (m = 2) were coated on themold of the Wolter mirror type I with a length of 20 cm,
and the Wolter supermirror was fabricated by using
replica method [4].
References[1] R. Maruyama et al., Physica B, Vol.385-86 1256-1258(2006).
[2] D. Yamazaki et al., JPS Conf. Proc. 8, 051009 (2015).
[3] H. Hayashida et al., Journal of Physics: Conference
Series 528 (2014) 012007.
[4] K. Soyama et al., Proc. 4th International Workshop on
Neutron Delivery Systems (2015).

D. Yamazaki1, R. Maruyama1, K. Soyama1, T. Miyauchi1, and H. Hayashida2
Neutron Insrumentation Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division, CROSS-Toka

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Large Area One-dimensional Scintillator Neutron
Detectors for TAKUMI at BL19
1. Introduction
The Engineering Materials Diffractometer, TAKUMIat BL19, is one of the neutron instruments installed at
the MLF of J-PARC. TAKUMI is designed specifically for
analysis of residual stress and crystallographic structureof industrial materials. The commissioning of TAKUMI
was started in September, 2008, and completed in
March, 2009. TAKUMI has been operated for more than
5 years with 10 detectors.
2. Neutron Detectors at TAKUMIThe neutron detectors installed at TAKUMI [1, 2] arelarge one-dimensional neutron detectors with a sensitive
area of 1 m × 20 cm and a position resolution of 3 mm, as
shown in Fig. 1, which have been developed under international collaboration with ISIS, Rutherford Appleton
Laboratory. The detectors were designed based on
those installed at the ENGIN-X instrument of ISIS. The
TAKUMI detector has 360 pixels, each with a size of 3 mm
× 20 mm, while the ENGIN-X detectors have 240 pixels
with a neutron sensitive area of 750 mm × 20 cm.

photomultiplier tubes (PMTs) and the electric signals
from the PMTs are sent to data acquisition electronics(DAE) and decoders. The position of the incident neutrons was determined by introducing 2Cn coding or apair-coded method in the arrangement of the fiber
bundle to PMTs, and hence each of the 360 pixels can be
specified by only 48 PMTs. The method also contributes
significantly to the noise reduction because the neutron
incident position is determined in the decoders by thecoincidence of the DAE output of any two PMTs. Anotherfeature of the detector is that the output count fromeach PMT has plateau characteristics, as shown in Fig. 2.
This is very favorable for setting the applied voltage.

Figure 2. Plateau characteristics of the PMT output count.

Figure 1. A Photograph of the neutron detector developed
for TAKUMI.

The detector head consists mainly of ZnS/6LiF scintillator, reflectors, and optical fibers. The scintillation
light generated as a result of nuclear reaction of 6Li withneutrons is efficiently collected into the optical fibersof the pixel, where the pixels are separated from eachother with a reflector. This “venetian” type head [3],originally developed by the ISIS facility, was adopted to
improve the efficiency of the light collection and neutron detection. The optical fibers are connected with

Last year these two types of detectors were fabricated and delivered to BL19, and thus a total of 12 detectors will be in service at TAKUMI. These detectors
have neutron sensitivity of more than 50% at 1 Å andgamma-ray sensitivity of less than 10−6 at a gamma-ray
energy of 1.3 MeV. The performances sufficiently meetthe requirements for residual stress analysis in the neutron scattering experiments at BL19.
References[1] K. Sakasai et al., Nucl. Instr. and Meth. A600 (2009)
157.
[2] K. Sakasai et al., Proc. of ICANS-XIX, (2010) IP131.
[3] E. M. Schooneveld and N. J. Rhodes, Proc. ICANS-XVI(2003) 455.

K. Sakasai, T. Nakamura, K. Toh, K. Honda, and K. Soyama
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center

124

MLF Annual Report 2014

Neutron Science

Development of Alternatives to the 3He Gas-based
Neutron Detectors in Nuclear Security
1. Introduction
The recent shortage of Helium-3 stockpiles severely
affected various fields such as neutron science and nuclear security. The US government established an initialstrategy for further allocation of the existing 3He supply. Consequently, in nuclear security, alternative technologies were encouraged and no further 3He gas wasallocated. Thus, it is quite urgent to develop a technology alternative to the conventional 3He gas-based neutron detectors in this field. Therefore, we have started
to develop alternative detectors with support from theJapanese government.
2. Developed Neutron Detector
The designed detector is shown in Fig.1. The detector has a simple design, comprising of a scintillator strip,
light-reflecting case, and two photomultiplier tubes(PMTs) at both ends [1, 2]. We have selected ZnS/10B2O3
ceramic scintillator as a neutron sensitive material,
which has been successfully adopted in detectors of
BL03, BL17, and BL18 at the MLF.

Figure 1. Photograph of the developed detector.

The scintillation light is generated in the scintillator
as a result of the nuclear reaction of 10B with neutrons
propagates to both ends of the case and then it is collected by the PMTs. The electrical signals from the two
PMTs are fed into inputs of the readout board which
was developed separately. Figure 2 shows a schematic
readout diagram of the detector. The electrical signals
from two PMTs are summed up by fast amplifiers andthe summed signal is again amplified and discriminated from background events in the board to obtain alogic signal as a neutron event.
In order to evaluate the detector performances

Figure 2. A schematic readout diagram of the detector.

objectively, demonstration experiments were conducted at the Facility of Radiation Standard, JAEA, inthe presence of three evaluators from IAEA, LANL, and
JRC (Joint Research Center). In the experiments, theneutron detection efficiency and gamma-ray sensitivityof our three detectors were precisely measured using a
252
Cf source and a 60Co source, respectively. The resultsof the experiments showed that the neutron efficiencyof the detectors was in the range between 74% and
80% and the gamma-ray sensitivity was less than 10−7
for all detectors. Here the neutron detection efficiency
is represented in a relative way, depending on the unit
length compared to that of a standard 3He neutron
counter (3He pressure: 4 atm, diameter: 1 inch). Notethat the gamma-ray sensitivity was measured undera high gamma-ray field of 100 mSv/hr. In such a highfield, a 3He-based neutron detector cannot be used because of pile-up of the gamma-ray pulses. These highperformances of the detectors were confirmed by thethree evaluators. The developed detector proved to be
one of promising alternatives to the conventional 3He
detectors used in nuclear security by this experiment.
This work was partially supported by the Ministryof Education, Culture, Sports, Science and Technology.
References[1] T. Nakamura et al., Proc. of 54th Annual Meeting of
the Institute of Nuclear Material Management.
[2] T. Nakamura et al., Nucl. Instr. and Meth. A763 (2014)
340.

K. Sakasai, T. Nakamura, K. Toh, H. Suzuki, K. Honda, and K. Soyama
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center

125Muon Scinece

Muon Scinece

MLF Annual Report 2014

Status of J-PARC MUSE
Because of the fire caused by the power supply
for the septum magnet at the muon D-line on January
16, 2015, we had to stop completely the operation of
J-PARC for one and a half months. Thanks to the tremendous efforts of the members of the J-PARC task force,the neutrino and neutron operations were restarted in
the end of February, 2015. Although we were about torestart the muon experiments in the end of April, wefaced a second trouble, a water leakage from the neutron target. According to the beam time schedule, wewill restart muon users’ RUN in the end of October.
1. Fire at the muon D-line
The fire at the Second Experimental Hall of theMaterials and Life Science Experimental Facility, J-PARC,
occurred at 15:01 on January 16, 2015. It happened in
the power supply for the septum magnet at the muon
D-line. To improve the stability of the current for the
septum magnet, an additional transformer was newly
fabricated and was going to be installed into the existing power supply. The installation work started on
January 7, 2015, and the electric power was energizedfor the first time on January 16. In a few minutes, after the circuit breaker was turned on, it was observedthat the transformer was smoking and burning locally.
Fortunately, the fire was put out by an extinguisher immediately, while calling 119 (emergency call). The causeof the fire was attributed to a miss-design of the circuitof the power supply, and specifically to the insufficient
safety check of the circuit, skipping the inspection by
the manufacturer under normal operation, as well as
the under-evaluation of the risk in the electrical power
test in the radiation control area by the J-PARC staff.
2. Installation of the rotating graphite target
Since September, 2008, we have been utilizing
safely and stably an edge-cooled non-rotating graphite target for the muon and pion production at J-PARC
MUSE. Considering the degradation of the thermal conductivity by the neutron irradiation, it was designed byinserting the buffer layer of the Ti interface between thegraphite and copper frame in order to release stress. So
far, proton beam intensity from the 3 GeV RCS has beenless than 300 kW, but it is planned to be upgraded up to
1.0 MW in one and a half years. Therefore, we decided toreplace the non-rotating target with a newly designed
rotating graphite target, which can accept proton beamwith much wider area, consequently reducing the128radiation damage. Its thickness, outer and inner diameter are 20, 330 and 230 mm φ. It is designed to be operated at 15 r.p.m. (rotations per minute) using WS2 solid
lubricant for the bearings, and its lifetime is expected
to be longer than 10 years, even in the 1 MW operation.
It has been operating stably without any trouble
since the beginning of November against 300 kW proton beam. Figure 1 shows a picture at the installation of
the muon rotating graphite target.

Figure 1. Installation of the muon rotating graphite target.

3. A new μSR spectrometer, KALLIOPE, at the D-Line
A new μSR spectrometer was installed at the D1
area. It consists of 1280 scintillators (640 telescopes)with their scintillation light detected by pixelled avalanched photo diodes (MPPCs), covering a total solid
angle of 23.4%, which is 3.3 times larger than theconventional D1 spectrometer, D-OMEGA1. The spectrometer, named KALLIOPE, is equipped with a 4-kG
Helmholtz coil with a gap of 135 mm, which can berotated by 90°, making it possible to apply eithertransverse or longitudinal magnetic field. It is also designed to be connected with a fly path chamber witha diameter of 410 mm. During the commissioning, it
was demonstrated that 200 M of coincidence positron
events per hour were collected for a sample specimenof 15 × 15 mm with a 20-mm collimator. The event rateis 2-3 times higher than that in ISIS-RAL, thanks to thestronger muon beam intensity of J-PARC.
We also installed a new dilution refrigerator at the
beginning of the users’ beam time for 2014B. Its features can be summarized in three points: 1) The cooling
period can be reduced to as low as 1.5 days without any
manpower by adopting an automatic cooling system;

MLF Annual Report 2014

2) Sample exchange can be done quickly by adopting a top-loading configuration; 3) No liquid helium
is required due to adopting a pulse-tube refrigerator.
Figure 2 shows a picture of the new dilution refrigerator
installed at the D1 spectrometer KALLIOPE.

Figure 2. Installation of a new dilution refrigerator for the D1
spectrometer.

4. The S-Line
We are constructing a new surface muon beamline dedicated to materials sciences research, called
the S-Line. Although eventually we are planning toconstruct four experimental areas, S1, S2, S3, and S4,
during this fiscal year we have received funding forconstruction of a beamline up to the S1 area. It consistsof large-acceptance quadrupole triplet magnets madeFigure 3. We passed the facility inspection radiation test in
November, 2014.

Muon Scineceof mineral insulation cables (MIC) as a front-end in thevicinity of the muon target, four sets of normal quadrupole triplet magnets and three sets of bending magnets
and an electrical kicker system, associated with a set of±250 kV DC separators.
Since we passed the facility inspection radiation test
in November, 2014, we are ready to perform beam line
commissioning. Figure 3 shows a picture of the S1 area.
5. U-LINE, the damaged window
At the U-Line, the front-end superconducting magnet in the superconducting curved solenoid, whichtransports intense surface muons efficiently from theproton beam line to the experimental area, had difficulties cooling down below the superconducting
temperature. A fiber telescope, inserted into the superconducting curved solenoid, revealed that the thermal
insulation window, designed to stop the heat radiation from the components at room temperature, wasbroken. In order to fix the damaged thermal insulation
window, we removed the shields in the vicinity of thesuperconducting curved solenoid, prepared a temporalradiation control area to prevent radioactive materials
from spilling out, and moved the curved solenoid fromthe primary tunnel to the experimental area in order to
fix it. In August, 2014, all repair works were completed
and we made sure that the device cooled down below
the superconducting temperature. Figure 4 shows apicture of the fixed thermal insulation window of thesuperconducting curved solenoid.

Figure 4. The damaged thermal insulation window was fixed
by removing all shields in the vicinity of the superconducting curved solenoid.

Y. Miyake1,2, N. Kawamura1,2, K. Shimomura1,2, P. Strasser1,2, A. Koda1,2, H. Fujimori1,2, S. Makimura1,2, Y. Kobayashi1,2, J. Nakamura1,2,
K. Nishiyama1,2, Y. Ikedo1,2, K. M. Kojima1,2, R. Kadono1,2, W. Higemoto2,3, and T. U. Ito2,3
1
Muon Science Laboratory, High Energy Accelerator Research Organization (KEK); 2Muon Science Section, Materials and Life Science
Division, J-PARC center; 3Advanced Science Research Center, Japan Atomic Energy Agency (JAEA)

129

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MLF Annual Report 2014

Installation and Operation of the Muon Rotating Target
1. Introduction
The muon production target is placed on the upstream of the neutron mercury target at J-PARC/MLF/
MUSE. A pulsed muon beam will be generated on amuon target made of 20-mm thick isotropic graphite.
The energy deposited by the 1-MW proton beam is estimated to be 3.9 kW on the muon target by PHITS. The firstmuon beam was successfully generated on September
26th, 2008. Gradually upgrading the beam intensity up
to 300 kW, the muon target with a fixed target method
has been used without replacement from the first muon
beam generation until May, 2014. Proton irradiation
causes radiation damage to the material properties ofgraphite. In particular, the effect on the graphite dimension is serious [1]. It is estimated that under the 1-MW
proton irradiation on graphite simulation, the lifetime of
the muon fixed target is 1 year. Because the muon target
is highly activated by proton irradiation, its handling after use must be performed at a remote handling room,
Hot cell. The remote controlled tasks require significant
time, cost and manpower. Therefore, the lifetime extension is essential for the stable operation of our facility.
To extend the lifetime, development of a muon rotatingtarget, in which the radiation damage is distributed toa wider area, began in 2008 in parallel with the proton
beam operation. While the lifetime of graphite becomeslong enough, the lifetime of the bearing becomes a critical issue. The development of the muon rotating target
has already been completed according to the resultsof analyses, detailed designs, and durability tests witha heating and rotating mock-up [2]. The muon rotating
was installed in September, 2014. Figure 1 shows pictures of the rotating target assembly on the left and therotating target on the lower-right. The schematic cutting
section is shown on the upper-right. A horizontal shaft,which is a rotation axis of the rotating target, is parallel tothe proton beam line. Because a motor device of the rotating target must be located 2.4 m above the beam line
level due to high radiation, the rotating motion is transmitted into the horizontal shaft through a vertical longshaft and a pair of bevel gears. The rotating body is composed of a graphite wheel, wheel support, and horizontal shaft supported by two horizontal bearings. The twobearings are attached to a cooling jacket in which water
piping is embedded. The outer and inner diameters of
the graphite wheel are 336 mm and 230 mm, respectively. The temperature of the graphite wheel was estimatedto be 940 K. The temperature of the hottest bearing was130

390 K. The rotation speed of the rotating target could bedetermined from the evaluation of the maximum temperature gradients inside the graphite. Consequently, it
was determined to be 15 rounds per minute (abbreviated as rpm afterwards). For the rotating target, bearings
supplied by JTEKT CO., LTD [3] were selected.

Figure 1. Pictures of the muon rotating target.

2. Bearing and solid lubricant
When the rotating target method is applied, the lifetime of the graphite will exceed 30 years. Then, the durability of the bearing will have a crucial impact on the
lifetime of the muon target. The bearings of the rotatingtarget are located in high vacuum of 10-4 Pa, at a hightemperature of 390 K, and under a high radiation dose of
100 MGy/year. Though disulfide molybdenum or silver isgenerally used in these conditions, the sintered compact
of disulfide tungsten is used for our target. Hereafter, disulfide molybdenum, silver, and disulfide tungsten areabbreviated as MoS2, Ag, and WS2 respectively. MoS2 or
Ag is coated on the components of the bearing, such asballs, inner ring, outer ring, and retainers. On the other
hand, the sintered compact of WS2 is inserted as separator of the balls. When WS2 is used, the quantity of the
lubricants is expected to be much larger than in thecase of MoS2 and Ag. Actually, according to the evaluation formula in the JTEKT catalogue, the lifetimes of ourbearings when using MoS2, Ag, and WS2 are 1100 hours,
5800 hours, and 110000 hours, respectively. The proton
beam has been actually operated for 5000 hours per

MLF Annual Report 2014

year. In the case of WS2, the lifetime of the bearings isestimated to be 22 years. However, it is not proven that
the WS2 could be used as a solid lubricant under a highradiation dose. Therefore, an irradiation test of WS2 byan electron beam was performed. In the irradiation
test, 80 [pieces of the sintered compacts of WS2 were
irradiated by a 2-MV, 1-mA electron beam in Takasaki
Advanced Radiation Research Institute, Japan Atomic
Energy Agency [4]. The estimate of radiation damage
caused to the pieces of WS2 was from 50 to 100 MGy. The
irradiated pieces of WS2 were assembled into 8 bearings.
Then durability tests under conditions similar to thoseat the beam line were performed in JTEKT. As a result,no irradiation effect was observed in the durability tests.
Figure 2 shows the pictures of the disassembled bearing
in the upper-left, the irradiation jig including only thecompacts of the solid lubricant in the upper-right, andthe electron-irradiation apparatus at the bottom.

Muon Scinece

transported by the shielding vessel, named muon transfer cask, and stored in the tentative storage pod at theLarge Apparatus Handling Room, which is located 10 m
above floor level [10]. Since the muon target assemblymust be kept in vacuum for corrosion control, suitablestorage vessels have been prepared. The muon fixed target, used for five years, was successfully replaced with a
new rotating target in September, 2014. Then, the usedmuon fixed target was activated at up to 400 mSv/hour
with 20-cm distance. The observation through remotecontrolled digital cameras did not register any cracks on
the target. Figure 3 shows pictures of the muon fixed target utilized for five years in the upper-left, the storage
vessels in the upper-right, and the replacement by themuon transfer cask at the bottom. Since then, the proton
beam operation by the muon rotating target has beensuccessfully performed without the increment of therotation-motor current. So far, the 300-kW and 400-kW
proton beam operation had been performed for threemonths. Furthermore, the 500-kW and the 600-kW operation had been performed for 2 weeks and for 1 hour,
respectively.

Figure 2. Pictures of the electron irradiation test of the solid
lubricants.

3. Installation and operation of the muon rotatingtarget
The muon fixed or rotating target is rigidly fabricated into the target rod. The target rod is integrated into
the plug shield through four screws, which can be handled remotely. The assembled components are called
target assembly. Because the muon target is highly activated by proton irradiation, the used muon target mustbe handled remotely. The used target assembly will be

Figure 3. Pictures of the replacement of the muon target.

References[1] H. Matsuo: Graphite 150 (1991) 290.
[2] S. Makimura et al., J. Radioanal. Nucl. Chem., DOI:
10.1007/s10967-015-3949-0.
[3] http://www.jtekt.co.jp/e/index.html[4] http://www.taka.jaea.go.jp/index_e.html

S. Makimura1, N. Kawamura1, S. Onizawa2, Y. Matsuzawa2, M. Tabe3, Y Kobayashi1, H. Fujimori1, Y. Ikedo1, A. Koda1, K. Kojima1,
Y. Miyake1, J. Nakamura1, K. Shimomura1, P. Strasser1, Y. Taniguchi1, and R. Kadono1
1
Muon Science Laboratory, J-PARC, High Energy Accelerator Research Organization (KEK); 2Nippon Advanced Technology Co., LTD (NAT);
3Seekel Co., LTD131

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MLF Annual Report 2014

Present Status of the D-Line
1. Replacement of the superconducting solenoid
magnet and the compressor
A conventional superconducting muon channel,
which can extract surface (positive) muons and decay
positive/negative muons up to 120 MeV/c, was operating successfully at the MLF experimental hall II before
the devastating earthquake of March 11th 2011. The superconducting solenoid magnet of 6 m of length consists of twelve units of 0.5 m coil. The magnet coil wasforced-indirectly cooled with supercritical helium gas(4.8 K at 0.80 MPaG) supplied by the on-line helium refrigeration system. The magnetic field was designed toreach a maximum of up to 5 T (current 730 A) at operational temperature of 6 K. The present magnetic field
for normal operation for surface/decay muon extraction is 0.308 T (45 A)/2.33 T (340 A), respectively
On-line helium refrigeration system was employed
to ensure the long-term stability of the operation.
The cooling power of the latter was 35 W at 4.5 K and
200 W at 80 K, and it was also able to produce 8 l/h ofliquid helium. The whole system was monitored andcontrolled by a VME controller, combined with a personal computer with dedicated software based on the
LabVIEW System, and cooled down automatically. The
typical cooling period from room temperature to operation temperature (~5 K) is about 3 days. Now thelong-term (typically 1 month) operation functions under quite stable conditions.
In FY 2010 the solenoid and the on-line refrigeration system operated smoothly for more than 5000 hrs
until the devastating earthquake on March 11th 2011.
On that day the system was operating, however, it was
stopped safely and no He gas was released. The damage
caused by the ground sinkage was serious, especially inthe on-line helium refrigeration system which became
unstable and the superconducting magnets also displayedfrequent instability under high current operations. Therefore we decided to replace these devices.
In FY 2014, the compressor of the on-line refrigeration system was replaced from Kaser to Mycom. Thus,
the cooling power of the on-line helium refrigeration
system was increased to 275 W at 4.5 K and to 400 W at
80 K, a new superconducting solenoid was also fabricated. This time we adopted warm bore type solenoid,
where no foils are needed to protect from thermal radiation. And the inner radius of the coils was increased from
12 cm to 20 cm. The changes are expected to improvedrastically the low energy muon (~100 keV) intensity.
132

Figure 1. Photograph of the new compressor (above) andthe solenoid (below).

2. Kicker system
The muon kicker system is used to separate themuon pulses and feed them simultaneously to two experimental areas (D1, D2). The beam operation with the
kicker system started successfully in the winter of 2011.
However, it was found that the ignition of the kicker
power supply produced kicker noise. The noise mainlycomprises a 10-MHz component that is dispersed into
the air, AC lines and detector signal lines. The kicker
noise level was drastically reduced by RF-shielding thetransmission lines with copper sheets and by reinforcing both the ground lines of the kicker system and thedetectors [1]. Employing bypass capacitors at the New
D1-μSR spectrometer was also successful [2]. However,further improvements are required for negative muonsand muonium experiments at the D2 area. Therefore,
electrically insulating the kicker chamber from the beamducts and its base, and reducing the ground impedancewere tested in this fiscal year. A plan to utilize a saturable
inductor for eliminating the noise is also described.
Copper plates were laid under the kicker oil tank to
reduce the ground (GND) impedance. The vacuum ducts
connecting to the kicker chamber at both ends were replaced with ceramic ducts in order to electrically insulate
the kicker chamber from the beam ducts and its base.

MLF Annual Report 2014

Muon Scinece

An outline of the kicker ground is shown in Fig. 2.
The kicker system was isolated from the beamline toprevent the noise through the ground line. The AC line
was also isolated from the other power lines with isolation transformers. Wide copper plates were used as low
impedance GND. However, these measures were notvery effective and actually increased the radiation noise.

while the rise-time of the kicker magnet current is kept
unchanged.

Figure 2. Outline of the kicker ground. Squares with pink line
denote the ceramic insulations.

Figure 3. Kicker system with saturable inductor.

The kicker noise source is the surge voltage at about
10 MHz that occurs with the ignition of the charged Pulse
Forming Network (PFN). So far we have taken measures
to protect the experimental signals against the surge
noise. A fundamental new measure, however, should betaken to remove the surge voltage at the output from
PFN. Bypassing the surge noise with capacitors could
be a possible solution. However, this method sacrifices
the rise-time of the kicker field instead. Alternatively, asaturable inductor (SI) was considered to eliminate thesurge without delaying the rise-time. The SI is made ofsaturable ferrite cores, and it functions as a large inductance at the onset of the surge voltage/current, then the
inductance decreases sharply due to the saturation of
ferrite as the current increases. In the circuit simulation
code, SPICE, the SI can be modeled as(

Lsat(I) = L0 Ae

−α I

)

+1

where L0 is the air-core inductance and I the current.
Two kinds of ferrite will be tested and their characteristics
are summarized in Table 1. The present parameters are
optimized for the initial charging voltage of PFN at 20 kV.
The diagram of the kicker system with the SI isshown in Fig. 3.
Figure 4 shows the result of the SPICE calculations.
It can clearly be seen that the surge current peaks
at both ends of the transmission line are eliminated,

Table 1. Parameter of the saturable inductors optimized for
20 kV operation.
Type
I
II

A
29.0
189.0

α
0.001171
0.002263

Bandwidth>80 MHz
12 MHzPower loss
12.5 W
2.6 W

Figure 4. Result of SPICE analysis for the case with (red) andwithout (blue) the SI. From top are shown the currents I1, I2 and I3 indicated in Fig. 3.

A kicker system directed single-pulsed muon beams
to the two existing experimental areas D1 and D2 simultaneously in March 2012. Now experiments with
the new spectrometer in the D1 area can be performed
with kicker-on without any noise problems. However,
the kicker noise level is still high for the experimentsin the D2 area. The trial with the saturable inductor isscheduled for September, 2015, in order to eliminate
the kicker noises at all relevant experimental areas.
References[1] H. Fujimori et al., KEK-MSL Report 2012 (2013) 16-17.
[2] H. Fujimori et al., KEK-MSL Report 2013 (2014) 20-21.

K. Shimomura1,2 and H. Fujimori1,2
1Muon Science Laboratory, High Energy Accelerator Research Organization (KEK), Tsukuba; 2J-PARC Center Cryogenics Section, Tokai

133

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MLF Annual Report 2014

U-Line; Lyman-α Laser Developments and Slow Muon
Beamline Commissioning
As it was mentioned in the previous report, the U-line
is one of the muon beamlines in the Material and Life
Science Experimental Facility of J-PARC, which provides
the world’s highest intensity of pulsed surface muons. It
was designed to produce ultra-slow muons through thethermal muonium laser resonant ionization method. The
ultra-slow muon beam is expected to be a new research
field in surface and interface physics. A new slow muon
beamline to supply ultra-slow muons is now under commissioning. The layout of the beamline is shown in Fig. 1.

krypton to generate 122.089 nm pulses. A coherent
212.556 nm light source for two-photon excitation anda tunable near-infrared light source are required in the
two-photon resonance four-wave mixing. The tunablenear-infrared light source is tuned around 820.649 and845.015 nm to generate VUV radiation at the muonium
Lyman-α resonance line and the hydrogen Lyman-αresonance line. In this fiscal year, we focused specificallyon the VUV generation at the hydrogen Lyman-α resonance line.

Figure 2. Optical system for two-photon resonance fourwave mixing [6]. Sodium salicylate and a photodiode, SXUV 300 were used for the observation of
Lyman-α resonance radiation and the determination of output energy, respectively.

Figure 1. The layout of the Ultra-Slow Muon Transport System.
F1~F5 show the focusing points of the beam line.

1. Developments of the laser system
Ultra-slow muons are generated in resonant ionization by the simultaneous irradiation of 122.089 nm,
which is the muonium Lyman-α resonance line and corresponds to the 1S-2P transition of the muonium atom,
and ultraviolet radiation at a wavelength of around
355 nm. Therefore, a high-energy coherent Lyman-αresonance radiation source is a critical element to efficiently produce ultra-slow muons.
Solid-state materials are not suitable for the generation of vacuum ultraviolet (VUV) radiation because they
are not transparent for a wavelength below 160 nm.
We chose two-photon resonance four-wave mixing in
134

Coherent light sources are required for the twophoton resonance four-wave mixing. The output pulses
at 212.556 and 845.015 nm were synchronized with theuse of an optical delay system and coaxially input to akrypton-argon gas cell for two-photon resonance fourwave mixing, as shown in Fig. 2. Although we obtained
3.2 and 1.6 mJ at 212.556 and 845.015 nm, the input
energies practically were restricted up to 0.8 and 1.5 mJ
at 212.556 and 845.015 nm because of optical losses inthe transmission system. Figure 3 shows the output energies at the hydrogen Lyman-α resonance line. While
Kr exhibits negative dispersion at vacuum ultra violet
wavelengths shorter than 124 nm, Ar exhibits positive
dispersion. Therefore, we have to mix Ar with Kr and control the mixture ratio of Ar and Kr for phase matchingin four-wave mixing. We adjusted the mixture ratio to
PAr/PKr ≈ 5 and changed the pressure from 0.02 × 103 toMLF Annual Report 2014

Figure 3. Output energy of coherent hydrogen Lyman-α resonance radiation (121.57 nm). 8.4 µJ in the gas celland 3.7 µJ at its outer side were obtained.

The conversion efficiency is an order of magnitude
higher than the one reported previously. The increaseof conversion efficiency is probably attributed to longer
interaction length and high-efficient mode matching infour-wave mixing caused by high beam qualities andthe same temporal profile of pump pulses.
In conclusion, we have accomplished a highconversion efficiency in two-photon resonancefour-wave mixing to generate Lyman-α resonanceradiation. Furthermore, we are currently developing
Nd:Y3Ga2Al3O12 ceramic power amplifiers to efficiently
increase the output energy up to 1 J at the fundamental
wavelength of 212.556 and 820.649 nm toward the realization of 100 μJ at 122.089 nm
2. Slow muon beam line tuning
In the previous fiscal year, almost all components of
the ultra-slow muon beam line were installed and the
optimization of the beam transportation was started byusing Li-ions.
In this fiscal year, we successfully transported Liions to μSR experimental port. Beam position and sizeare estimated by using slits and Micro Channel Plates(ROENDEC DLD40) at each focusing point. The results ofthe measurements are shown in Fig. 4 and Table 1.

Table 1. Li-ion beam width in sigma at each focusing point.
Position
F1
F2
F3
F4A
F5A

Horizontal Width
1.2 mm
3.8 mm
1.0 mm
3.8 mm
2.9 mm

Vertical Width
1.3 mm
4.1 mm
2.1 mm
4.0 mm
6.4 mmFigure 4. An example of measured beam distribution. A horizontal distribution of the Li-ions at F3. Dots show
the measured particle late and red lines show thefitted gauss function.

For tests of the laser system and better tuning of
the beamline, hydrogen atoms are ionized by laser andtransported as a pilot beam. The laser ionized hydrogens
are successfully transported to the μSR experimental
port. The measured time of flights (TOF) between the laser injections and the particle detections agree with thecalculated TOF of the hydrogen ion, as shown in Fig. 5.
The tuning of the beamline is currently underway
for the first ultra-slow muon beam at J-PARC.
This work was supported by MEXT KAKENHI Grant
Number 23108002.
10Time of flight [μs]3.20 × 103 Pa. When the pressure was approximately 2.20
× 103 Pa, the output energy at the hydrogen Lyman-αresonance line increased up to 8.4 μJ in the gas cell. The
output energy corresponds to a conversion efficiency of
3.6 × 10−3 (≈ 8.4 × 10−6 J / [1.5 × 10−3 J + 0.8 × 10−3 J]).

Muon Scinece

D+ (calc)
H+ (calc)
μ+ (calc)

5

Measurement

0
0

5000

10000

15000

Path Length [mm]Figure 5. Time of flight of the beam. Dots show the results ofthe measurements. Lines show the calculated TOFof the deuterium-ion, hydrogen-ion and muon.

T. Adachi1,2, Y. Ikedo1,2, J. Nakamura1,2, A. Yabuuchi1,2, P. Strasser1,2, Y. Oishi3, N. Saito4, K. Miyazaki4, K. Okamura4, S. Wada4,
T. U. Ito2,5, W. Higemoto2,5, K. M. Kojima1,2, K. Shimomura1,2, R. Kadono1,2, Y. Miyake1,2, M. Iwasaki3, and E. Torikai61Muon Science Laboratory, High Energy Accelerator Research Organization (KEK); 2Muon Section, Materials and Life Science Division,
J-PARC centre; 3Advanced Meson Science Laboratory, RIKEN Nishina Center for Accelerator-Based Science (RNC); 4Photonics Control
Technology Team, RIKEN Center for Advanced Photonics (RAP); 5Advanced Science Research Centre, Japan Atomic Energy Agency (JAEA);
6Interdisciplinary Graduate School of Medicine and Engineering, University of Yamanashi

135Muon Scinece

MLF Annual Report 2014

Construction of the Muon S-Line and Installation of theGeneral Purpose μSR Spectrometer
1. Introduction
The surface muon beamline (S-Line) in experimental hall No.1 of the Materials and Life science experimental Facility (MLF) building is designed to provide
low-energy muon beam, which is mainly utilized by materials and life science experiments (Fig. 1). Following
the construction of the power supply yard and the concrete shields completed in the previous fiscal year [1],the primary goal of the project in 2014 was the installation of the beamline components.

equipment continued along with the installation, because some of the assembled equipment included a
few devices manufactured by independent companies. In the case of the electric kicker, for example, thevacuum chamber and electrodes were made by Irie
Koken Co., Ltd., the switch-yard magnet and the magnetic end-guards were made by NEC Tokin Corp., andthe high-voltage pulse transformer was made by Pulse
Power Japan. Fig. 2 shows that the main components ofthe electric kicker situated at the beamline height, suchas the vacuum chamber and the pulse transformers, canbe integrally manipulated after being assembled, since
they are carried on the upper stage of the kicker support. This part, which is detachable from the lower support frame, is installed in the beamline with sufficient
reproducibility by using guiding pivots. The scheme
mentioned above is also helpful to conduct some installation tasks simultaneously, such as anchoring supports on the floor, assembling devices, and alignment
along the beamline axis.

Figure 1. Beamline layout of the S-Line (phase1).

2. Cooling water
Soon after the MLF shutdown in July, the concrete
shields were removed to install cooling water pipes
along the beamline magnets. In order to reduce thenumber of the pipes passing through the piping duct of
the concrete shield, one triplet quadrupole magnet, e.g.
SQ7-8-9, uses a common water pipe to control the total
flow rate. To cope with the change in the flow balanceamong quadrupole magnets, a small water manifoldwith three controlling valves to distribute cooling water
is situated near the magnet. Besides, three power supplies connected to each of the triplet quadrupole magnets monitor a common flow switch activated in caseof problems with the water supply. In addition to this,the status of each quadrupole magnet is monitored
by two devices: a differential pressure switch and thermal switches attached to hollow conductors. The same
monitoring devices are installed for SQ4-5-6, which isplaced in the primary beam tunnel.
3. Beamline equipment assembly
The final assembling and testing of the beamline
136

Figure 2. Assembling the electric kicker. One of the pulse
transformers is about to be attached to the vacuum
chamber.

4. Installation of the beamline components
In the beginning of September, 2014, most of thebeamline components were successfully installed andthe major task at this stage was to place cables. On
the other hand, due to a technical problem during thepressure test of the cooling water pipe, the operationof the magnets and the power supplies for adjustment
was suspended. After discussions among the task force
organized by the MLF division members, the coolingMLF Annual Report 2014

system was restarted in mid-October. Finally, the facility inspection on November 7, 2014, confirmed that the
Muon S-Line was operating successfully.
5. General-purpose spectrometer
As reported elsewhere [2], we have designed andinstalled a general-purpose μSR spectrometer (0.4 Tesla
longitudinal field coil with capability of accepting various sample environment inserts) at the D1 experimental
area. In FY2014, we manufactured another general-purpose spectrometer with Element Strategy grant. Its design is identical to that of the D1 spectrometer, and is to
be installed at the S1 experimental area (Fig. 3).

magnetic field vectors measured at four points aroundthe sample. The feedback system actively achieves <0.4 μTesla stray field at the sample position.
Table I. specification of D1/S1 μSR spectrometer.
Magnets
Longitudinal field BZ(//beam)
LF magnet bore and gap
LF homogeneity
LF stability
Transverse field By(⊥beam, vertical)
TF homogeneity
TF stability
Correction field coils forzero-field (CCBx, y, z)
CF homogeneity
Positron Counters
Number of channels
Detector solid angle

Sample insert
bore and the gap

Figure 3. General-purpose μSR spectrometer installed at theS1 experimental area.

The specifications of the D1/S1 spectrometer are
listed in Table I. It is equipped with a 0.4 Tesla longitudinal field (Bz) coil and a 14-m Tesla transverse-field coil(By), both of which are normal conducting magnets.
The stability and the homogeneity of the magnetic
fields are shown in Table I. The zero-field correction coils
are driven by an active feedback system based on the

Muon Scinece

Maximum 0.4 Tesla(1000 amps, 100 V)
ø400, 135 mm
0.1% ø20 mm, 1% ø50 mm
Drift < 0.01% for 8 hours
Ripple Vp-p < 0.01%
Maximum 14-m Tesla(100 amps, 40 V)
0.1% ø20 mm, 1% ø50 mm
Drift < 0.05%
Ripple Vp-p < 0.1%
Maximum 1-m Tesla(10 amps, 20 V)
0.5% ø20 mm, 10% ø50 mm
32ch × 40 Kalliope units =1280 channels (640 pairs)
21.2% of 4π(2 × 8 array of 10 × 12 mm
scintillator cubes: covers
1920 mm2 area at 180 mm
and 161 mm from sample)
ø254, 135 mm

The positron detectors are 40 Kalliope units eachof which has 32 sets of 10 × 10 × 12 mm cubic scintillators [1]. The total number of the individual positroncounters is thus 40 × 32 = 1280 channels (640 coincidenced pairs) covering 21.2% of the 4π solid angle.
The count rate and the spectrum features have to
wait for the beam commissioning of the S1 experimental area, starting in FY2015.
References[1] A.Koda et al., KEK-MSL Annual report (2013).
[2] K. M. Kojima et al., J. Phys: Conf. Ser., 551 (2014)
012063, (2014); K. M. Kojima et al., KEK-MSL Annual
report (2013).

A. Koda1,2, P. Strasser1,2, K. M. Kojima1,2, N. Kawamura1,2, H. Fujimori1,2, K. Nishiyama1,2, and J-PARC Muse staff
1
Muon Science Laboratory, High Energy Accelerator Research Organization(KEK); 2Muon Section, Materials and Life science Division,
J-PARC Center

137

Muon Scinece

MLF Annual Report 2014

Present Status of the H-Line
The construction of a brand new 4th beam line, theH line, has been planned for MUSE. The new beam line
is designed to have a large acceptance, momentum
tunability, and the ability to use kicker magnet andWien filter. This beam line will provide an intense beamfor experiments which require high statistics and need
to be conducted for relatively long periods in the experimental areas. Several experiments in the field offundamental physics studies have been proposed for
the H line [2-4].
From the existing muon production target at MUSE,
it is possible to extract 4 muon beam lines. The H line isextracted to the south east direction in experimental
hall #1.

every passing year. According to the evaluation usinga Monte-Carlo code [5], the dose rate beside the target chamber was estimated to be close to 1 Sv/h, andthe summer shutdown in 2012 was the ultimate time
limit to install the frontend magnets in the H line. Thus,
the installation of the frontend devices was completed
mainly in 2012 and partially in 2014, as shown in Fig. 2
and 3.

HB1

HGV1

φ600 pillow seal

HS1a

HS1b

Figure 2. Installed frontend devices in the H line.

H lineH1 exp. area

HB2

S lineFigure 1. A layout plan of experimental hall #1 in the firstphase.

In the initial stage of the MUSE construction, only
the D line and the front-end magnets in the S line were
installed, consequently the front-end magnets in the
U line were installed in 2009. Temporary radiationshield blocks were placed in the H line. J-PARC has been
operating since 2008, so the activation around themuon production target becomes more serious with
138

Figure 3. Picture taken after the installation of the frontend
devices in the H line was completed.

In the other high intensity beam line in MUSE, theU line, we adopted only axial focusing magnets to obtain high transmission efficiency [6]. On the other hand,in the H line, the beam captured by an axial focusinglarge-aperture solenoid magnet is transmitted throughbending magnets, although these non-axial focusing
magnets increase the beam loss. To compensate for this

MLF Annual Report 2014

and improve the high transmission efficiency, large aperture magnets and other devices have been adopted
in the H line. A typical size of the aperture is 600 mm indiameter.
The conceptual design work of the major components in the experimental hall, i.e. magnets, vacuum
components and so on, is almost converged for the firstphase of the H line in which the beam line is constructed to the first experimental area, as shown in Fig. 1.
At present, the detailed mechanical design work is inprogress. In order to provide sufficient muon beam to
all planed experiments in the H line, the design work is
performed with the participation of the collaborators in
the proposed experiments. For instance, the g-2/EDM
experiment [3], for which the beam line is extended
straight through the bending magnet (HB2), needs tofocus the surface muon beam on the muonium production target which will be placed several tens of centimeters apart from the exit of the last magnet. The beam
spot size is required to be as small as possible. In addition, the magnetic field in the muonium production
target is required to be smaller than 1 mT, and thus theleakage field of the beam line magnet generally is not
negligible. To satisfy these requirements, after HB2 thesurface muons are transported and semi-focused by asolenoid magnet (HS4), and then focused on the muonium target by quadrupole magnets [7].

Muon Scinece

concrete shield will be necessary to enclose the streaming neutrons and other radiation sources. Because the
H line adopts large aperture devices, the effects of thestreaming neutrons are more serious than in the case ofother beam lines. The evaluation of the streaming neutrons is important not only for radiation safety but also
to check their effect on the detectors and other devices
in the experimental area. Figure 5 shows a typical result of the simulation. While the proton beam is on, thedose rate in the experimental area is expected to reach
100 μSv/h, and no one can enter into the area even if nobeam is delivered. By inserting a beam blocker, which isa 40-cm thick copper block, the dose rate is reduced bya factor of ten. Both the beam blocker and the switching off of HB2 guarantee the personnel safety against
radiation, and comprise the personal protection interlock system.
(a) blocker out(b) blocker in

100 μSv/h

10 μSv/h

blocker

Figure 5. A typical simulated result of the radiation dosearound the H line. To enter the experimental area,
a beam blocker was inserted in the right while noblocker was used in the left.

Figure 4. Final focusing part for the g-2/EDM branch.

The radiation shield design proceeds according to the method previously applied at the otherbeam lines [5]. Along the beam line, a few-meter thick

References[1] N. Kawamura et al., 2013 Journal of Physics:
Conference Series 408 012072.
[2] K. Shimomura et al., ibid.
[3] N. Saito et al., ibid.
[4] S. Mihara et al., ibid.
[5] N. Kawamura et al., 2009 NIM A 600 114.
[6] K. Nakahara et al., 2010 AIP Conf. Proc. 1222 420.
[7] A. Yoyoda et al., 2013 Journal of Physics: Conference
Series 408 012073.

N. Kawamura1,2, MuHFS collab., DeeMe collab., and g-2/EDM collab.
1Muon Science Section, Materials and Life Science Division, J-PARC; 2Muon Science Laboratory, High Energy Accelerator Research
Organization (KEK)139

MLF Safety

MLF Safety

MLF Annual Report 2014

Research Safety
1. Radiation safety(Improvement of shielding estimation)
From the construction stage of MLF, shields of only
each beamline (single-beamline-model) were considered as the shielding estimation. However, because theproton beam-power increases and many beamlines
with their shields have been constructed, the shielding
estimation with the single-beamline- model is not realistic and is over spec. Therefore, shields of all the beamlines (all-beamline model) were proposed as the newshielding estimation method and adopted in the new
application of the radiological license. Figure 1 shows
an example of the all-beamline-model for the shielding
estimation [1].

Figure 1. Example of the all-beamline-model for the shielding estimation at the 2nd experimental hall.

(Measurement of shielding performance of all neutron
beamlines)
In order to apply the 1 MW operation in the radiological license, we measured dose rates at outside of theshields of the all neutron beamlines with the 300 kW
proton beam operation.
As the results, it was confirmed that it was enoughshielding performance at almost beamlines. However,it was found that there was not enough shielding performance at several beamlines with only a specific case.
Therefore, shields of such the beam lines were estimated by the shielding calculation and several shields
were added. Finally enough low dose rates could be
confirmed by the measurement.
142(Radiological license upgrade)
Normally, we have two chance of the application
on radiological license upgrade in a year.
In the first application, the radiological license waspermitted on Sep.9, 2014, and was updated for the following items:(1) Installation of the neutron beam line BL22,(2) Minor change to the shielding configuration
for preparation of installation of the muon
beam line (H line),(3) Extension of controlled area and addition of
one entrance to it at the BL09 building.
In the second application, the radiological license
was permitted on Dec. 11, 2014, and was updated forthe following items:(4) Upgrade the maximum proton beam power induced to MLF from 2.6 × 1018 proton/h (350 kW)
to 7.5 × 1018 proton/h (1 MW),(5) Improvement of the shielding estimation
method (The all-beamline-model was adopted. )(6) Extension of controlled area for completion of
the experiment preparation building.
By this permission, the 1 MW proton beam operation at MLF became available as the license.
The neutron beam line BL06 and the muon beamline S line are available because the two beam lines
passed the facility inspection in 2014.
2. Chemical safety
For neutron and muon experiments, a lot of chemical substances have been brought into and used in
MLF. The checking-in process, usage and storage ofchemicals such as solid, gas and liquid are managed by
the chemical safety group. Figure 2 shows an annualchange on the number of experimental samples whichwere submitted for MLF proposals and safety-checkedby using sample risk assessment sheets.
In particular, the chemical safety group makes assessments of the handling of highly toxic chemicals,
and requires extra care which may cause serious injury.
Chemicals are stored safely in cabinets and on shelvesin an upright position. Chemical fume hoods are surveyed annually by the group. Chemical fume hood velocities for all hoods on MLF are evaluated on an annual
basis by Facilities.

MLF Annual Report 2014

MLF Safety

operated, inspected, and maintained by the machinesafety group. Pre-use, monthly, and annual inspection
are conducted according to the J-PARC center safety
instructions. Figure 3 shows a monthly change on thenumber of times of crane use.

Figure 2. Annual change on the number of experimental
samples which were safety-checked.

3. Electrical safety
For safety check of a lot of electrical equipment, internal regulations based on governmental regulations
and appropriate standards are applied to prevent hazard and damages in MLF. The number of user’s devices
safety-checked by the electrical safety group was 289
on the 2014A and 334 on the 2014B proposal.
In particular, safety interlock system is required forexperimental devices. For example, an overcurrent protective circuit is required for an electrical power supply
and so on in order to prevent fire and injuries caused byelectricity include electrical shock and burns.
Fuses and circuit breakers, which are safety devices
that protect equipment from high currents or voltages
and prevent overheating of electrical wires, are periodically safety-checked by the electrical safety group using
meggers.
4. Machine Safety
In each experimental hall at MLF, 7.5 ton craneand 30 ton crane are under operation. These are

Figure 3. Monthly change on the number of times of craneuse.

The total number of times of use of cranes in 2014is 215. Those were mainly used by inside operators, but
the 52 was used by outside company’s operators. The
machine safety group safety-checked how to use thecranes and slings about all of proposals.
For safety check of laser equipment used for neutron and muon experiments, internal regulations basedon the Japanese Industrial Standards Committee (JIS)is applied. Technical reviews of 4 equipment were conducted in 2014A and 2014B at MLF by the special committee on laser.
Reference[1] Application of the radiological license (attachedreference material for MLF), permitted on Dec.11,
2014, (2014).

M. Harada1, M. Ooi1, M. Sekijima1, T. Kai2, Y. Kasugai5, K. Aizawa3, S. Ono3, H. Tanaka3, W. Kambara3, Y. Ito3, M. Nakamura2, K. Suzuya2,
S. Makimura4, Y. Sakaguchi6, and T. Yamashita6
1
Neutron Source Section; 2Neutron Science Section; 3Technology Development Section; 4Muon Science Section, Materials and Life Science
Division, J-PARC Center; 5Radiation Safety Section, Safety Division, J-PARC Center; 6Neutron R&D Division, CROSS-Tokai

143

MLF Operations in 2014

MLF Operations in 2014

MLF Annual Report 2014

CROSS-Tokai 2014 Update
The Public Neutron Beam Facility at J-PARC
Consistent with its longstanding policy of promoting open access to major publicly-funded research facilities, the Japanese government established in July2009 the Public Neutron Beam Facility at J-PARC. The
Facility consists of the accelerators and target station
used to generate pulsed neutron beams and a proportion of the beamlines that exploit the neutron beams
for research purposes.
The legislative framework within which the Public
Neutron Beam Facility was established requires that an
independent third-party organization be responsible
for the administration and support of the science program on the so-called ‘Public Beamlines’. CROSS-Tokai
was appointed to this role and began operations fromits offices in the Ibaraki Quantum Beam Research Centeradjacent to the J-PARC site in early 2011.
Although CROSS-Tokai is structurally independentof JAEA and KEK – the co-owners and operators of
J-PARC – it maintains a high level of cooperation andcollaboration with the two founding organizations andother stakeholders that is driven by shared scientificobjectives.

terms, can be summarized as follows: Manage proposal selection and beamtime allocation
 Provide user support and ancillary experimental
facilities
 Provide assistance and expert advice to existing andpotential users
 Initiate and undertake outreach and facility utilization promotion activities Manage the selection and assessment of Contract
Beamlines
The Public Beamlines at J-PARC MLF
The MLF has capacity to accommodate up to 23
neutron beamlines around the present target station.
There are currently 18 neutron and 2 muon beam instruments in operation, 2 neutron instrument in commissioning and 2 new beamlines under construction.
Of these, 6 beamlines have been designated as Public
Beamlines as part of the Public Neutron Beam Facility
and are supported by CROSS-Tokai.
Though not exhaustive in their experimental capabilities, the Public Beamlines cover a wide range ofneutron scattering techniques and can be used in a variety of research fields. The Public Beamlines at J-PARC
MLF are listed in Table 1 with examples of their research
applications.

The Role of CROSS-TokaiCROSS-Tokai is entrusted with specific responsibilities relating to the Public Beamlines which, In practical

3GeV Synchrotron

Materials & Life Science
Exptl Facility

Hadron Exptl Facility

Neuclear Transmutation
Exptl Facility (Planned)(Muon-Neutron)
Linac
50GeV Synchrotron
Neutrino Exptl Facility

Areas of J-PARC covered by the Promotion of Public Use legislation
Figure 1. The Public Neutron Beam Facility at J-PARC (shown in red).

146

MLF Annual Report 2014

MLF Operations in 2014

Table 1. The Public Beamlines at J-PARC MLF.

Number

Instrument

Applications

BL01

4SEASONS – 4D-Space Access
Neutron Spectrometer

Lattice and spin dynamics in condensed matter over a wide range of 4D
momentum-energy space

BL02

DNA – Biomolecular Dynamics
Spectrometer

Atomic and spin dynamics of biological macromolecules soft matter andfunctional biomaterials

BL11

PLANET – High-Pressure Neutron
Diffractometer

Structural analysis and radiography of materials under extreme pressure
and temperature

BL15

TAIKAN – Small and Wide Angle
Neutron Scattering Instrument

Nano and micro scale structural analysis of metals, magnetic materials,
soft matter and bio-macromolecules

BL17

SHARAKU – Polarized Neutron
Reflectometer

Structural analysis of functional and magnetic thin films, biological thinfilms and buried interfaces

BL18

SENJU – Extreme Environment
Single Crystal Diffractometer

Microcrystalline and magnetic structural analysis of functional materials

BL22
RADEN- Energy-Resolved Neutron
in commissioning Imaging System

Visualization of the spatial distribution of crystal structures, nuclides
and magnetic domains by neutron transmission imaging and 3D
reconstruction

Distribution of Beamtime on the Public Beamlines
The Selection Committee of CROSS-Tokai regularly
reviews and sets policies for the distribution of beamtime on the Public Beamlines at the MLF. In line withthe prescribed role of the Public Beamlines and taking into account operational requirements, beamtime
is currently distributed in approximately the following
ratios:(a) General Use(d) Director’s Discretion (up to 5%)(b) Elements Strategy Initiative (up to 15%)(e) CROSS-Tokai Research (up to 15%)

(C) Trial Use (up to 5%)(f )Facility Use (up to 25%)

Figure 2. Beamtime Distribution on the Public Beamlines.

CROSS-Tokai in 2014
Overview
After four years of operation, CROSS-Tokai is now
fully engaged in the full range of its mandated activities: proposal selection via an open and transparent
assessment process, provision of high-quality user support, and facility utilization promotion within both theacademic and industrial research sectors.
At the start FY2014, CROSS-Tokai was supporting the user program on six fully-operational Public
Beamlines: BL01 4SEASONS, BL02 DNA, BL11 PLANET
BL15 TAIKAN, BL17 SHARAKU and BL18 SENJU. BL22
RADEN had been prepared as the 7th Public Beamline
and will be available to users in 2015. For informationon the current status and science programs on the

Public Beamlines, please see the individual beamline
updates in Chapter 3 of this Report.
As the number of Public Beamlines at the MLF
continues to increase, and with strong growth in user
demand for beamtime, CROSS-Tok0ai has continued to
grow as an organization. During FY2014, the total number of CROSS-Tokai staff rose to 62 with five team members being employed: all of them in the Neutron R&D
Division and working in direct support of the science
program on the beamlines.
The Public Beamlines hosted during FY2014, experiments associated with over 250 research proposals andCROSS-Tokai continued to vigorously promote facility
utilization both in Japan and internationally.

147

MLF Operations in 2014

MLF Annual Report 2014

CROSS-Tokai 2014 Highlights
 Dr. Yokomizo became the Director of CROSS-Tokai.
On 1 June 2014, Dr. Hideaki Yokomizo became
the second Director of CROSS-Tokai, succeeding Prof.
Yasuhiko Fujii who so ably served in this role for morethan three years since CROSS-Tokai began operations in
support of the Public Neutron Beam Facility at J-PARC.

 Trial Use
An important part of CROSS-Tokai’s work in promoting the utilization of the Public Beamlines is to grow theuser community – particularly among industry-based
researchers – through outreach and education activities. In addition, from 2012B, CROSS-Tokai has been operating the Trial Use Access Program that aims to assist
novice users of neutron-based techniques gain experience and expertise that will allow them to become independent General Use applicants in the future.
The specific objectives of the Trial Use Access
Program are:
 To grow the user community and,
 To promote the use and utility of pulsed neutrons through the development and demonstration of innovative new applications

Figure 3. An acceptance speech by Director Yokomizo.

 Commissioning of RADEN to begin user operations
as the 7th Public Beamline from 2015
From April 1, 2015, BL22 RADEN will become theseventh Public Beamline at the MLF and will be madeavailable for user operations for the first time in 2015A.
CROSS-Tokai is proceeding with preparatory work
for starting user operations from April 2015 in cooperation with J-PARC.
With the addition of RADEN, the range of scientificfields that can be undertaken on the Public Beamlines
has been extended to include the study of visualizationof the spatial distribution of crystal structure, nuclides
and magnetic domains by neutron transmission imaging and 3D reconstruction.
For more information about RADEN and its capabilities, please see the detailed beamline update in
Chapter 3 of this report.

Figure 4. A flight tube (Front) and a detector (rear) in RADEN
measuring room.

148

Accordingly, up to a maximum of five percent (5%)
of the total beamtime on each of the Public Beamlines
at the MLF can be allocated for Trial Use experiments ineach round.
Employing the specialist expertise and experienceof the CROSS-Tokai Science Coordinators and other appropriate staff, the Trial Use system offers support toprospective users through the whole process of facility
utilization including: Instrument selection and experiment feasibility assessment
 Proposal preparation
 Experiment design, planning and execution
 Data analysis and interpretation
 Publication of results
The Trial Use program continued to gather paceduring Fy2014 with expressions of interest comingfrom organizations in the industrial and academic sectors. Ultimately, 11 projects were developed into full
beamtime proposals and approved by the Selection
Committee. A list of the Trial Use proposals approved
in FY2014 is given in Table 2. It is particularly pleasing
to note the diversity of science and the high degree ofacademia-industry collaboration that is being encouraged and supported by the Trial Use program.
We look forward to describing in future reports,scientific outcomes from the Trial use program as wellas the return of Trial use applicants in future rounds as
General Users.

MLF Annual Report 2014

MLF Operations in 2014

Table 2. Trial Use proposals approved inFY2014.

Round

2014A

2014B

Beamline

Industry

Research Area

BL01 4SEASONS

Toyota Motor Corporation

Automotive

Thermoelectric Materials

BL02 DNAIBARAKI University.

University

CementBL15 TAIKANJSR Co.

Chemicals

Polymer

BL15 TAIKANDNP FINE CHEMICALS Co., Ltd.

Chemicals

Pigment

BL01 4SEASONSTokyo Institute of Technology

University

Phase Transitions

BL02 DNAFC-Cubic

Battery

Fuel Cell

University

Carbon Fiber†

BL11 PLANET

Shinshu University

BL15 TAIKAN

Nagoya Institute of Technology

University

Gel

BL15 TAIKAN

Toray Research Center, Inc.†

Analysis Service

Polymer

Electric equipment

Film

University

Organic Material

BL17 SHARAKU
BL18 SENJU†

Applicant organization

KONICA MINOLTA䠈 Inc.

††Tokyo Metropolitan University

TU experiments approved by the Selection Committee but not carried out due to the Muon facility incident.

Other Key CROSS-Tokai activities FY2014
 Proposal Selection
 Public Beamlines proposal selection for 2014B
 Call for Proposals (Jun-Jul 2014) – 128 proposals submitted
 Review by Expert Panels and Proposal
Evaluation Committee (31 July-1 Aug,2014)
 Selection Committee (21 Aug 2014) – 74
proposals approved (incl. 7 Trial Use and 2
Proprietary Use) Public Beamlines proposal selection for 2015A
 Call for Proposals (Oct-Nov 2014) – 118
proposals submitted
 Review by Expert Panels and Proposal
Evaluation Committee (16, 19-20 Jan -2014)
 Selection Committee (27 Jan 2015) – 75
proposals approved (incl. 6 Trial Use and 2
Proprietary Use)

Figure 5. Public beamlines proposal selection for 2014B (Selection Committee, 21 Aug 2014).



CROSS Development Proposal Evaluation
Panel (25-26 Dec 2014) – 3 one-year proposals
approved for FY2015.

 User Support
CROSS-Tokai is now supporting user operations
and ongoing instrument development activities on
the six Public Beamlines with a Neutron R&D team of
38 scientists, programmers, engineers and technicians. Table 2 shows by type and operation period, thenumber of research proposals supported on the Public
Beamlines during FY2014.
In addition to our work at the beamlines, CROSSTokai continues to develop and maintain ancillary user
facilities in the Ibaraki Quantum Beam Research Center
including: User Experiment Preparation Laboratories I(Sample processing), II (Hard Matter) and III(Soft Matter & Biomaterials).
 User Data Analysis Room
 User Lounge and “Refresh Rooms”
 Outreach and Facility Promotion
Throughout FY2014, CROSS-Tokai has continued toengage in a wide variety of outreach and facility utilization promotion activities. Both independently and incollaboration with other stakeholders in the neutron science community, CROSS-Tokai convened or otherwise
supported in more than 20 events designed to informnew potential users about the research possibilities ofneutrons, disseminate the latest research results andexperimental capabilities and build opportunities forcollaboration with other large-scale research facilities.
149MLF Operations in 2014

MLF Annual Report 2014

Table 3. Research proposals supported on the Public Beamlines in FY2014.

2014A
2014B

Full year

BL01

BL02

BL11

BL15

BL17

BL18

TOTAL

GU

13

9

11

16

14

7

70

TU

1

1

0

2

0

0

4

GU

12

12

8

15

11

9

67

TU

1

1

1

2

1

1

7

ESI

1

0

0

3

1

0

5

DP

0

1

0

0

0

2

3

PU

3

3

0

5

1

3

15

Instrum.

1

1

1

1

1

1

6

32

28

21

44

29

23

177

TOTAL

GU: General Use
DP: CROSS Development Proposals

TU: Trial Use
PU: JAEA Project Use

ESI: Element Strategy Initiative
Instrum: Instrument Group Proposals

User Experiment Preparation
Laboratory I

User Experiment Preparation
Laboratory II

User Experiment Preparation
Laboratory III

User Data Analysis RoomUser Lounge

Refresh Rooms

Figure 6. User facilities in the Ibaraki Quantum Beam Research Center.

Highlights of these activities in 2014 included:
 Promotional booths at local and international
conferences The CROSSroads Workshop Series
 Industrial Applications workshops and user
meetings
 Complementary Use workshops

150

Research presentations at local and international scientific meetings
For a comprehensive summary of workshops, symposiums, seminars, etc. hosted or supported by CROSSTokai in 2014, please see the full listing of events in
Chapter 6 of this report.

MLF Annual Report 2014

MLF Operations in 2014

Beam Operation Status at MLF
In Japanese Fiscal Year (JFY) 2014, the beam operation at the MLF started with a beam power of 300 kW.
Figure 1 shows the trend of the beam power and theaccumulation of beam power during JFY2014. For theaccelerator study, a high power beam of up to 1 MW operated in January, 2015, for several shots of beam.

the front end of the LINAC such as the ion source and
RFQ were replaced to produce 1 MW beam. After theexchange of the mercury target of the MLF, a relatively
stable beam operation was performed with 300 kW
beam until the end of December. In early January, several shots of beam with 1 MW equivalent beam power
were successfully delivered to the mercury targets. On
January 16th, a fire incident occurred at the power supply for the muon decay line and as a result the beam
operation at Run #60 was completely canceled. After
recovering from the incident, a beam operation has
started with 400 kW beam power. Although the beam
was stopped for 5 days from February 28 to March 4 because the cryogenic system had to be recovered, a relatively high beam availability was achieved. The overall
record for JFY2014 shows that about 70% availability
was achieved, and the down period was caused mainlyby the beam loss during Run #60.

Table 1. Run cycle, scheduled time and availability.
Figure 1. Beam power trend (shown in blue line) at MLF
and cumulative beam power (shown in red line) in
JFY2014.

Table 1 shows the scheduled time and availability.
In JFY2015, we had a good start with relatively highavailability in Run #53. During Run #54, a lower availability such as 52% was caused by trouble with thechoke transformer of the RCS. Up to end of June, arelatively high availability with 300 kW beam operation
was achieved. During the summer shutdown period,

Run #
53
54
55
56
57
58
59
60
61
OverallDate
Apr 1 – 7
Apr 14 – May 1
May 2 – Jun 3
Jun 4 – Jun 26
Nov 1 – Nov 25
Nov 29 – Dec 22
Jan 17 – Feb 17
Feb 18 – Mar 31

Scheduled Availability
Time (h)
(%)
151
89.7
382
52.2
718
91.1
488
87.4
nouse
478
79.6
466
96
646
0
790
76.1
4119
69.1

151

MLF Operations in 2014

MLF Annual Report 2014

Users at the MLF
After a long shutdown of the accelerator operation
due to an incident at the Hadron Facility, the operation
was resumed in January, 2014. Therefore, the combined
number of neutron and muon users at the MLF in fiscal
year 2014 was the largest ever recorded. On the other
hand, there were fewer foreign users of the muon instruments than in the previous fiscal year, which may

have been a result of the shutdown of the muon-beam
operation due to a fire of a power supply in the muon
experimental hall, which occurred in January, 2015. The
transition of the number of users at the MLF is summarized in Table and Figure for domestic and foreign usersof neutron and muon experimental facilities.

Table 1. The number of Japanese and foreign users in the period of fiscal year.
FY2008FY2009FY2010FY2011FY2012FY2013

FY2014

Japanese Foreigners Japanese Foreigners Japanese Foreigners Japanese Foreigners Japanese Foreigners Japanese Foreigners Japanese Foreigners
Neutron
Muon

182
161

378
21

353

12
12

529
25

485

57
0

55

222
44

198

55
2

48

735
24

650

30
7

28

520
85

452

72
2

62

Neutron (Japanese)

Neutron (Foreigners)

Muon (Japanese)

Muon (Foreigners)

68

2

10

62

12

55
25

21

353

FY 2009
200
2
09

88

62
85

69

650
485

161

FY 200
2008
08

10

48
44

FY 2010
20
010

2
28
24
198

FY 2011
20
011
1

15
62
68

755

15

88

900
750

45
450
300
30

452

150
15
FY 201220
012

0FY 2013201
13FY 2014
4

69
91

60
600

Figure 1. The number of Japanese and foreign users in the period of fiscal year.

152

755

77

3

7

824

3

MLF Annual Report 2014

MLF Operations in 2014

MLF Proposals Summary – FY2014
Table 1. Breakdown of Proposals Numbers for the 2014A & 2014B Rounds.
2014A
Beam-line

Instrument

2014B

Full Year

Submitted

Approved

Submitted

Approved

Submitted

GU

GU

GU

GU

PU/S

IU

ES PU/S

Approved
IU

ES

BL01

4D-Space Access Neutron Spectrometer - 4SEASONS

20 (1)

14 (1)

17 (1)

13 (1)

3

1

1

3

1

1

BL02

Biomolecular Dynamics Spectrometer - DNA

18 (1)

10 (1)

23 (1)

13 (1)

3

2

0

3

2

0

(100-β)‡

6

2

8

2

0

0

0

0

0

0

†

0

0

0

0

15

0

0

9

0

0

6

6

12

10

1

1

0

1

1

0

BL03

Ibaraki Biological Crystal Diffractometer - iBIX

BL04

Accurate Neutron-Nucleus Reaction Measurement Instrument ANNRI

BL05

Neutron Optics and Physics - NOP

5

2

3

1

1

0

0

1

0

0

BL08

Super High Resolution Powder Diffractometer - S-HRPD

15

8

14

10

1

0

1

1

0

1

BL09

Special Environment Neutron Power Diffractometer - SPICA

0

0

0

0

1

0

0

1

0

0

BL10

Neutron Beamline for Observation and Research Use - NOBORU

21

10

26

11

2

1

0

2

1

0

BL11

High-Pressure Neutron Diffractometer - PLANET

14

11

9 (1)

9 (1)

0

1

0

0

1

0

(β)

BL12

High Resolution Chopper Spectrometer - HRC

95

12 (2)

8 (2)

1

0

0

1

0

0

BL14

Cold-neutron Disk-chopper Spectrometer - AMATERAS

21

7

29

9

2

1

2

2

1

2

BL15

Small and Wide Angle Neutron Scattering Instrument - TAIKAN

37 (2)

18 (2)

40

15

5

1

3

5

1

3

BL16

High-Performance Neutron Reflectometer with a horizontal
Sample Geometry - SOFIA

11

10

7

7

1

0

0

1

0

0

BL17

Polarized Neutron Reflectometer - SHARAKU

20

14

12 (1)

12 (1)

1

1

1

1

1

1

BL18

Extreme Environment Single Crystal Neutron Diffractometer SENJU

24

725 (1)

10 (1)

3

3

0

3

3

0

BL19

Engineering Diffractometer - TAKUMI

25

15

28

13

3

1

2

3

1

2
0

(100-β)

‡

16

7

9

9

0

0

0

0

0

14

14

7

7

14

0

0

13

0

0

High Intensity Total Diffractometer - NOVA

21

13

14

8

1

0

1

1

0

1

D1

Muon D121(1)16 (1)

34 (2)

16 (2)

0

1

0

0

1

0

D2

Muon D2

1110

13 (1)

9 (1)

0

1

0

0

1

0

U

Muon U

BL20

Ibaraki Materials Design Diffractometer - iMATERIA

BL21

Total

(β)‡

0

0

0

0

1

0

0

1

0

0

335

199

342

192

59

15

11

52

15

11

GU : General Use
PU : Project Use or Ibaraki Pref. Project Use
S : S-type Proposals
IU : Instrument Group Use
ES : Element Strategy† : Ibaraki Pref. Exclusive Use Beamtime (β = 80% in FY2014)‡ : J-PARC Center General Use Beamtime (100-β = 20% in FY2014)( ) : Proposal Numbers under Trial Use Access System or P-type proposals (D1,D2) in GU

153

MLF Operations in 2014

MLF Annual Report 2014

800
700
293

600
Proposals

142

278

500

Not Approved

400

Approved

42
300

45

20
200

309

34
67

214

FY2008FY2009

100

460

422

469

FY2012FY2013

FY2014255

0FY2010FY2011

Proposal Round
Figure 1. MLF Proposal Numbers over Time.

KEK, 24,
4%

Universies (Japan)
Companies (Japan)

JAEA, 104, 16%
Foreign Organizaons,
ganizaons,
88, 13%

Research Instutes (Japan)
Universies (Japan),
300, 46%

Foreign Organizaons
JAEA
KEK

Research Instutes (Jaapan),1, 11%
71
Companies (Japan),69, 10%Figure 2. Origin of Submitted Proposals by affiliation - FY2014.

Q1, 26, 4%
P9, 11, 2%
Q2, 50,8%
P1, 152, 23%

P7, 43,43 7%
P6, 58, 9%

P2, 38, 6%

P5, 169, 26%

P3, 98, 15%

P1 : Materials Science and Engineering
P2 : Energy ScienceP3 : Soft Matter, Biomaterials and Liquids
P4 : (Reserved)
P5 : Magnetism and Strongly Correlated Electron Systems
P6 : Fundamental Physics, Nuclear Science and Instrument R&D
P7 : Industrial Applications
P8 : (Reserved)
P9 : Trial Use Access Program
Q1 : Electronic Properties of Matter
Q2 : Hydrogen in Matter & General Applications

Figure 3. Origin of Submitted Proposals by Sub-committee/Expert Panel – FY2014.

154

MLF Annual Report 2014

MLF Operations in 2014

MLF Division Staff 20142014 General Meeting of MLF (7 July, 2014)

Head

Masatoshi Arai

Deputy Head

Hideki Seto
Masatoshi Futakawa

Neutron Source Section*: additional duties<JAEA>
Hiroshi Takada (Leader)

Tetsuya Kai*

Motoki Ooi

Yoshimi Kasugai (Sub-Leader)

Yuuko Kato

Kenji Sakai

Katsuhiro Haga (Sub-Leader)

Yoshihiko Kawakami

Masakazu Seki

Atsushi Akutsu

Tomoyuki Kawasakii

Hideki Tatsumoto

Katsuhiro Aoyagi

Ohtsu Kiichi

Makoto Teshigawara

Tomokazu Aso*

Hidetaka Kinoshita

Toshitsugu Uchida

Masahide Harada

Hiroyuki Kogawa

Hideki Ueno

Shoichi Hasegawa*Shin-ichiro Meigo

Takashi Wakui

Mitsunori Hirane

Hideki Muto

Zhihong Xiong

Miyuki Hoshino

Takashi Naoe

Shizuka Yoshinari

Masato Ida

Norio Narui

Usamah Zaid Shahrul BashahKenji Imahashi

Masaaki Nishikawa

Hideaki Ishii

Ken-ichi Oikawa*

155

MLF Operations in 2014

MLF Annual Report 2014

Neutron Science Section*: additional duties<JAEA>
Kenji Nakajima (Leader)

Ryoichi Kajimoto

Ken-ichi Oikawa

Yukinobu Kawakita (Sub-Leader)

Wataru Kambara*

Asami Sano*

Kazuya Aizawa*

Kouji Kaneko*

Mariko Segawa*

Kazuhiro Aoyama

Seiko Kawamura

Kaoru Shibata

Satoru Fujiwara*

Takuro Kawasaki

Naoko Shimizu

Hideo Harada*

Naoko Kawase

Takenao Shinohara

Masahide Harada*

Tatsuya Kikuchi

Yuhua Su

Stefanus Harjo

Atsushi Kimura*

Kentaro Suzuya

Takanori Hattori

Ryoji Kiyanagi

Shin-ichi Takata

Kousuke Hiroi

Satoshi Kunieda*

Masayasu Takeda*

Tomonori Hosoya

Kazuo Kurihara*

Tarou Tamada*Hiroshi Iikura*

Futoshi Minato*

Itaru Tamura*

Yasuhiro Inamura

Hiroshi Nakagawa*

Chiho Tobe

Takaaki Iwahashi

Mitsutaka Nakamura

Yousuke Tou*

Nobuyuki Iwamoto*

Shoji Nakamura*

Shuichi Wakimoto*Tetsuya Kai

Takashi Ohhara

Masao Watanabe*

Shinichi Ito (Sub-Leader)Takashi Ino

Kaoru Taketani

Hideki Seto

Takashi Kamiyama

Shuki Torii

Hitoshi Endo

Naokatsu Kaneko

Norifumi Yamada

Haruhiro Hiraka

Kenji Mishima

Tetsuya Yokoo

Soshi Ibuka

Hidetoshi Oshita

Masao Yonemura

Kazutaka Ikeda

Toshiya Otomo<KEK>

Technology Development Section*: additional duties<JAEA>
Kazuya Aizawa (Leader)

Yoshimi Kasugai*

Kaoru Sakasai*

Takayuki Oku (Sub-Leader)

Hiroyuki Kogawa*

Kentaro Suzuya*

Tomokazu Aso

Kentaro Moriyama

Shin-ichi Takata*

Chikako Doda

Mitsutaka Nakamura*

Hiromichi Tanaka

Wu Gong

Tatsuya Nakamura*Kazue Tanaka

Katsuhiro Haga*

Takeshi Nakatani

Masao Watanabe

Yukihiro Ito

Motoki Ohi*

Yasuhiro Yamauchi

Tetsuya Kai*

Shino Ono

Wataru Kambara

Kenji Sakai*

<KEK>

156

Tomohiro Seya

Naritoshi Kawamura*

Setsuo Sato

Hiroshi Fujimori*

Kenji Kojima*

Kaoru Taketani*

Takashi Ino*

Shunsuke Makimura*

Shuki Torii*

Naokatsu Kaneko*

Masataka Sakaguchi

Testuya Yokoo*

MLF Annual Report 2014

Neutron Instrumentation Section

MLF Operations in 2014*: additional duties<JAEA>
Kazuhiko Soyama (Leader)

Katsunori Honda

Kaoru Sakasai

Noriko Amezawa

Ryuji Maruyama

Hiroyuki Suzuki

Kentaro Fuji

Tatsuya Nakamura

Dai Yamazaki

Hirotoshi Hayashida

Takurou Sakai*

Ryo Yasuda*

Muon Science Section*: additional duties<KEK>
Yasuhiro Miyake (Leader)

Yasuo Kobayashi

Hirotaka Okabe

Taihei Adachi

Akihiro Koda

Koichiro Shimomura

Hiroshi Fujimori

Kenji Kojima

Patrick Strasser

Koji Hamada

Shunsuke Makimura

Masato Tabe

Masatoshi Hiraishi

Masanori Miyazaki

Soshi Takeshita

Li HuaJunpei Nakamura

Yutaka Taniguchi

Yutaka Ikedo

Yohei Nakatsugawa

Motonobu Tanpo

Ryosuke Kadono

Yasuhisa Nemoto

Atsushi Yabuuchi

Naritoshi Kawamura

Kusuo Nishiyama

Ichihiro Yamauchi<JAEA>
Wataru Higemoto*Takashi Ito*

157

MLF Operations in 2014

MLF Annual Report 2014

CROSS-Tokai Staff 2014

Farewell party for Director Fujii (27 May, 2014)

Director

Yasuhiko Fujii (Until May, 2014)
Hideaki Yokomizo (From June, 2014)

Science Coordinators
Masatoshi Sato

Yoshiaki Fukushima

Neutron R&D Division158

Jun-ichi Suzuki (Head)

Satoshi Kasai

Koji Munakata

Kenichi Funakoshi (Head (Deputy))

Yukihiko Kawamura

Akiko Nakao

Jun AbeHiroshi Kira

Masashi Obinata

Kazuhiro Akutsu

Koji Kiriyama

Kazuki Ohishi

Takayasu Hanashima

Makoto Kobayashi

Keiichi Ohuchi

Hirotoshi Hayashida

Tetsuya Kuroda

Nobuo Okazaki

Hideyuki Hiramatsu

Shinichi Machida

Joseph Don PARKER

Kazuki Iida

Yoshihiro Matsumoto

Masae Sahara

Kazuhiko Ikeuchi

Masato Matsuura

Yoshifumi Sakaguchi

Motoyuki Ishikado

Noboru Miyata

Taiki Tominaga

Takayoshi Ito

Tazuko Mizusawa

Takeshi Yamada

Hiroki Iwase

Toshiaki Morikawa

Shuoyuan Zhang

Kazuya Kamazawa

Taketo MoyoshiMLF Annual Report 2014

Health and Safety Division
Toshiyuki Yamashita (Head)MLF Operations in 2014*: additional duties

Rei Ohuchi*

Koji Kiriyama*

Yukihiko Kawamura*

Utilization Promotion Division
Junichi Sato (Head)

Ritsuka Ishikawa

Emi Takaha

Garry John FORAN (Head (Deputy))

Megumi Kawakami

Hiroyuki Takasaki

Toshiki Asai

Junko Ohta

Aya Yamada

Yutaka Ebara

Rei Ohuchi

Shinichi Yamaguchi

Asami Inoue

Sayaka Suzuki

Admin and Finance Division
Yasuo Seishi (Head)Mika Gunji

Mutsumi Shiraishi

Masaru Yokoyama (Head (Deputy))

Takashi Hikita

Tomoyuki Yabana

159

MLF Operations in 2014

MLF Annual Report 2014

Proposals Review System, Committees and Meetings

Proposal Review System
The JAEA-KEK-CROSS Agreement of Cooperaon on the Promoon of Public Ulizaonof the Speciﬁc Neutron Beam Facilies at J-PARC (Enacted on 1 April 2011)
President
JAEA

Director General
KEK

J-PARC
Center(JAEA/KEK)

President
CROSS
CollaboraonCommiee

Director
J-PARC

Director
CROSS-Tokai

All except Public Beamlines

Muon Instrument
Proposal Rev. Comm.

Muon Science
Proposal Rev. Comm.

Selecon
Commiee

Task Forces

All except Public
Beamlines

Public Beamlines Only

Neutron Science
Proposal Rev. Comm.

Proposal
Evaluaon Comm.

Contract Beamlines
Only

Neutron Instrument Contract Beamline
Proposal Rev. Comm. Evaluaon Comm.
Joint Meeng

Muon
Instrument
Proposals(CROSS)

Public Beamlines Only

MLF Advisory
Board

All except Contract
Beamlines

RegisteredInstuon

Joint Meeng

Neutron Instrument
Proposals

Public Beamlines Only
All except Public Beamlines
Neutron Program
JAEA Research
CROSS Development
Advisory
Proposal Advisory Proposal Evaluaon
CommieeCommiee
Panel
Joint MeengMuon Program
Advisory Comm.

Muon Scienﬁc Proposals

Neutron Scienﬁc Proposals
UniﬁedAccess Point

ALL Proposals submied via the J-PARC Users Oﬃce
Figure 1. Proposals Review System Framework.

Materials and Life Science Facility Advisory Board

Jun Sugiyama

Toyota Central R&D Labs., Inc., Japan

Jun Akimitsu

Aoyama Gakuin University, Japan

Yasuhiko Fujii

Koichiro Asahi

Tokyo Institute of Technology, Japan

Comprehensive Research
Organization for Science andSociety, Japan

Mikio Kataoka

Nara Institute of Science andTechnology, Japan

Masatoshi AraiJapan Atomic Energy Agency, Japan

Toshiji Kanaya

Kyoto University, Japan

Takashi KatoJapan Atomic Energy Agency, Japan

Masatoshi Futakawa

Japan Atomic Energy Agency, Japan

Kazuya Aizawa

Japan Atomic Energy Agency, Japan

Masayasu Takeda

Japan Atomic Energy Agency, Japan

Taku Sato

Tohoku University, Japan

Mitsuhiro Shibayama The University of Tokyo, Japan(Chair)
Kyoto University, Japan

Yukinobu Kawakita

Japan Atomic Energy Agency, Japan

Makoto Hayashi

Ibaraki Prefectural Government,
Japan

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Toshio Yamaguchi(Deputy Chair)

Fukuoka University, Japan

Takashi Kamiyama

High Energy Accelerator Research
Organization, Japan

Masahiko Iwasaki

RIKEN, Japan

Toshiya Otomo

Youji Koike

Tohoku University, Japan

High Energy Accelerator Research
Organization, Japan

Masaaki Sugiyama

160

MLF Annual Report 2014

Yasuhiro Miyake

High Energy Accelerator Research
Organization, Japan

Ryosuke KadonoHigh Energy Accelerator Research
Organization, Japan

Shinichi Itoh

High Energy Accelerator Research
Organization, Japan
Term: through March 31, 2015

Neutron Instrument Proposal Review Committee
Koichiro Asahi

Tokyo Institute of Technology, Japan

Muneyuki Imafuku

Tokyo City University, Japan

Kenji Ohoyama

Tohoku University, Japan

Hideaki Kitazawa

National Institute for Materials
Science, Japan

Yoshiaki Kiyanagi

Nagoya University, Japan

Mamoru Sato
Jun-Ichi Suzuki

MLF Operations in 2014

Yukinobu Kawakita

Japan Atomic Energy Agency, Japan

Toshiya Otomo

High Energy Accelerator Research
Organization, Japan

Brendan Kennedy

The University of Sydney, Australia

Sergey Danilkin

Australian Nuclear Science andTechnology Organisation, Australia

Masaaki Sugiyama

Kyoto University, Japan

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Toshio Yamaguchi

Fukuoka University, Japan

Mamoru Sato

Yokohama City University, Japan

Sung-Min Choi

Korea Advanced Institute of Scienceand Technology, Korea

Michael James

Australian Synchrotron, Australia

Paul Langan

Oak Ridge National Laboratory,
U.S.A

Yokohama City University, Japan

Shinichi Shamoto

Japan Atomic Energy Agency, Japan

Comprehensive Research
Organization for Science andSociety, Japan

Masatoshi AraiJapan Atomic Energy Agency, Japan

Takahisa Arima

The University of Tokyo, Japan

Naoya Torikai

Mie University, Japan

Shinichi Itoh

Yukio Morii

Radiation Application Development
Association, Japan

High Energy Accelerator Research
Organization, Japan

Masaaki Matsuda

Yukio Morimoto

Kyoto University, JapanOak Ridge National Laboratory,
U.S.A

Hideki Yoshizawa

The University of Tokyo, Japan

Je-Geun Park

Seoul National University, Korea

Masatoshi AraiJapan Atomic Energy Agency, Japan

Masatoshi Futakawa

Japan Atomic Energy Agency, Japan

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Kenji Nakajima

Japan Atomic Energy Agency, Japan

Takashi Kamiyama

High Energy Accelerator Research
Organization, Japan

Toshiya Otomo

High Energy Accelerator Research
Organization, Japan
Term: through March 31, 2015

Neutron Science Proposal Review Committee
Yoshiaki Akiniwa

Yokohama National University,
Japan

Yukio Noda

Tohoku University, Japan

Jun-Ichi Suzuki

Comprehensive Research
Organization for Science andSociety, Japan

Seung-Hun Lee

University of Virginia, U.S.A

Hirohiko M. Shimizu

Nagoya University, Japan

Yuji Kawabata

Kyoto University, Japan

Yasuhiro Miyake

High Energy Accelerator Research
Organization, Japan

Albert Young

North Carolina State University,
U.S.A

Guinyun Kim

Kyongpook University, Korea

Koichi Akita

Japan Atomic Energy Agency ,Japan

Yukio Morii

Radiation Application Development
Association, Japan

Makoto Hayashi

Ibaraki Prefectural Government,
Japan

Yoshiaki FukushimaComprehensive Research
Organization for Science andSociety, Japan
Term: through March 31, 2017

Masatoshi Futakawa

Japan Atomic Energy Agency, Japan

Neutron Program Advisory Committee

Hiroyuki Kagi

The University of Tokyo, Japan

Koichiro Asahi

Tokyo Institute of Technology, Japan

Samrath Chaplot

Bhabha Atomic Research entre,
India

Kazuaki Iwasa

Tohoku University, Japan

Anna Paradowska

Australian Nuclear Science andTechnology Organisation, Australia

Masaki Azuma

Tokyo Institute of Technology, Japan

Mikio Kataoka

Yasushi Idemoto

Tokyo University of Science, Japan

Nara Institute of Science andTechnology, Japan

Takashi Kamiyama

High Energy Accelerator Research
Organization, Japan

Toshiji Kanaya

Kyoto University, Japan

Michihiro Furusaka

Hokkaido University, Japan161

MLF Operations in 2014

MLF Annual Report 2014

Yasushi Idemoto

Tokyo University of Science, Japan

Shinichi Shamoto

Japan Atomic Energy Agency, Japan

Hiroshi Kageyama

Kyoto University, Japan

Kenji Nakajima

Japan Atomic Energy Agency, Japan

Masaaki Sugiyama

Kyoto University, Japan

Yukinobu Kawakita

Japan Atomic Energy Agency, Japan

Moritomo Yutaka

University of Tsukuba, Japan

Mitsuhiro Shibayama The University of Tokyo, Japan
Hirohiko M. Shimizu

Nagoya University, Japan

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Toshiya Otomo

High Energy Accelerator Research
Organization, Japan

Ryosuke KadonoHigh Energy Accelerator Research
Organization, Japan

Muon Instrument Proposal Review Committee
Koichiro Asahi

Tokyo Institute of Technology, Japan

Nobuhiko Nishida

Tokyo Institute of Technology, Japan

Masahiko Iwasaki

RIKEN, Japan

Yoshitaka Kuno

Osaka University, Japan

Kenya Kubo

International Christian University,
Japan

Hiroyuki Nojiri

Tohoku University, JapanRIKEN, Japan

Reiji Kumai

High Energy Accelerator Research
Organization, Japan

Yasunori Yamazaki
Masatoshi AraiJapan Atomic Energy Agency, Japan

Noboru Yamamoto

High Energy Accelerator Research
Organization, Japan

Takashi KatoJapan Atomic Energy Agency, Japan

Youichi MurakamiHigh Energy Accelerator Research
Organization, Japan

Masatoshi Futakawa

Japan Atomic Energy Agency, Japan

Toru Ogitsu

High Energy Accelerator Research
Organization, Japan

High Energy Accelerator Research
Organization, Japan

Ryosuke KadonoHigh Energy Accelerator Research
Organization, Japan

High Energy Accelerator Research
Organization, Japan

Kenji Kojima

High Energy Accelerator Research
Organization, Japan

Koichiro Shimomura

High Energy Accelerator Research
Organization, Japan

Yasuhiro Miyake

High Energy Accelerator Research
Organization, Japan

Wataru Higemoto

Japan Atomic Energy Agency, Japan

Takashi Kamiyama
Shinichi Itoh

Term: through March 31, 2015

JAEA Research Proposal Advisory Committee
Toshiya Otomo

High Energy Accelerator Research
Organization, Japan

Hiroyuki Kagi

The University of Tokyo, Japan

Toshiji Kanaya

Kyoto University, Japan

Yuji Kawabata

Kyoto University, Japan

Hideaki Kitazawa

National Institute for Materials
Science, Japan

Yoshiaki Kiyanagi

Nagoya University, Japan

Takashi Sakuma

Ibaraki University, Japan

Hirohiko M. Shimizu

Nagoya University, Japan

Jun-Ichi Suzuki

Comprehensive Research
Organization for Science andSociety, Japan

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Yo Tomota

Ibaraki University, Japan

Masaki Fujita

Tohoku University, Japan

Takatsugu Masuda

The University of Tokyo, Japan

Youichi MurakamiHigh Energy Accelerator Research
Organization, Japan

Koichi Akita

162

Term: through March 31, 2017

Japan Atomic Energy Agency ,Japan

Masatoshi AraiJapan Atomic Energy Agency, Japan

Takashi KatoJapan Atomic Energy Agency, Japan

Yukinobu Kawakita

Japan Atomic Energy Agency, Japan

Term: through March 31, 2015

Muon Science Proposal Review Committee
Hiroshi Amitsuka(Chair)Hokkaido University, Japan

Masatoshi AraiJapan Atomic Energy Agency, Japan

Kazuyoshi Yoshimura Kyoto University, Japan
Seiji Miyashita

The University of Tokyo , Japan

Ryosuke KadonoHigh Energy Accelerator Research
Organization, Japan

Reiji Kumai

High Energy Accelerator Research
Organization, Japan

Yoji Koike

Tohoku University, Japan

Yoh Kohori

Chiba University, Japan

Yasuo Nozue

Osaka University, Japan

Wataru Higemoto

Japan Atomic Energy Agency, Japan

Kenji Kojima

High Energy Accelerator Research
Organization, Japan

Takashi Kamiyama

High Energy Accelerator Research
Organization, Japan

Alan Drew

University of London, U.K.

Koichiro Asahi (Chair) Tokyo Institute of Technology, Japan

MLF Annual Report 2014

MLF Operations in 2014

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Kenji Kojima

High Energy Accelerator Research
Organization, Japan

Toshiji Kanaya

Kyoto University, Japan

Koichiro Shimomura

Shinji Tsuneyuki

The University of Tokyo , Japan

High Energy Accelerator Research
Organization, Japan

Kenya Kubo

International Christian University,
Japan

Yoko Sugawara

Kitazato University, Japan

Toshiya Otomo

High Energy Accelerator Research
Organization, Japan

Tadashi Koseki

Term: through March 31, 2015

Selection Committee (CROSS)
Toshio Akai

Mitubishi Rayon co.,Ltd., Japan

High Energy Accelerator Research
Organization, Japan

Jun Akimitsu

Aoyama Gakuin University, Japan

Koichiro Asahi

Tokyo Institute of Technology, Japan

Masaharu Aoki

Osaka University, Japan

Mikio Kataoka

Yasuyuki Matsuda

The University of Tokyo , Japan

Nara Institute of Science andTechnology, Japan

Yuichiro Nagame

Japan Atomic Energy Agency, Japan

Toshiji Kanaya

Kyoto University, Japan

Koichiro Shimomura

High Energy Accelerator Research
Organization, Japan

Shin-Ichi Kamei

Mitubishi Reserch Institute, Inc.,
Japan

Roderick Macrae

Marian University, U.S.A, Japan

Naoki Kishimoto

Yasuhiro Miyake

High Energy Accelerator Research
Organization, Japan

National Institute for Materials
Science, Japan

Taku Sato

Tohoku University, Japan

Mitsuhiro Shibayama The University of Tokyo, Japan
Term: through March 31, 2015

Muon Program Advisory Committee

Masaaki Sugiyama

Kyoto University, Japan

Masaki Takada

RIKEN, Japan

Kiyoyuki Terakura

National Institute of Advanced
Industrial Science and Technology,
Japan

Kazumi Nishijima

Mochida Pharmaceutical co.,Ltd.,Japan

Makoto Hayashi

Ibaraki Prefectural Government,
Japan

Hidetoshi Fukuyama

Tokyo University of Science, Japan

Toshio Yamaguchi

Fukuoka University, Japan

Masaharu Aoki

Osaka University, Japan

Koichiro Asahi

Tokyo Institute of Technology, Japan

Hiroshi Amitsuka

Hokkaido University, Japan

Masatoshi AraiJapan Atomic Energy Agency, Japan

Toshiji Kanaya

Kyoto University, Japan

Kenya Kubo

International Christian University,
Japan

Youji Koike

Tohoku University, Japan

Yoh Kohori

Chiba University, Japan

Yoko Sugawara

Kitazato University, Japan

Shinji Tsuneyuki

The University of Tokyo , Japan

Proposal Evaluation Committee (CROSS)

Yasuo Nozue

Osaka University, Japan

Yoshiaki Akiniwa

Yokohama National University,
Japan

Yukio Noda

Tohoku University, Japan

Jun-ichi Suzuki

Comprehensive Research
Organization for Science andSociety, Japan

Hiroyuki Kagi

The University of Tokyo, Japan

Samrath Chaplot

Bhabha Atomic Research entre,
India

Anna Paradowska

Australian Nuclear Science andTechnology Organisation, Australia

Yasushi Idemoto

Tokyo University of Science, Japan

Brendan Kennedy

The University of Sydney, Australia

Sergey Danilkin

Australian Nuclear Science andTechnology Organisation, Australia

Masaaki Sugiyama

Kyoto University, Japan

Term: through March 31, 2015

Kazuyoshi Yoshimura Kyoto University, Japan
Wataru Higemoto

Japan Atomic Energy Agency, Japan

Yasuyuki Matsuda

The University of Tokyo , Japan

Seiji Miyashita

The University of Tokyo , Japan

Hideki Seto

High Energy Accelerator Research
Organization, Japan

Toshiya Otomo

High Energy Accelerator Research
Organization, Japan

Ryosuke KadonoHigh Energy Accelerator Research
Organization, Japan

Reiji Kumai

High Energy Accelerator Research
Organization, Japan

Tadashi Koseki

High Energy Accelerator Research
Organization, Japan

Yasuhiro Miyake

High Energy Accelerator Research
Organization, Japan

Toshio Yamaguchi

Fukuoka University, Japan

Mamoru Sato

Yokohama City University, Japan163

MLF Operations in 2014

MLF Annual Report 2014

Sung-Min Choi

Korea Advanced Institute of Scienceand Technology, Korea

Michael James

Australian Synchrotron, Australia

Paul Langan

Oak Ridge National Laboratory,
U.S.A

Takahisa Arima

The University of Tokyo, Japan

Masaaki Matsuda

Oak Ridge National Laboratory,
U.S.A

Je-Geun Park

Seoul National University, Korea

Seung-Hun Lee

University of Virginia, U.S.A

Hirohiko M. Shimizu

Nagoya University, Japan

Yuji Kawabata

Kyoto University, Japan

Albert Young

North Carolina State University,
U.S.A

Guinyun Kim

Kyongpook University, Korea

Yukio Morii

Radiation Application Development
Association, Japan

Makoto Hayashi

Ibaraki Prefectural Government,
Japan

Yoshiaki FukushimaComprehensive Research
Organization for Science andSociety, Japan
Term: through March 31, 2017

CROSS Development Proposal Evaluation Panel
Hiroyuki Kagi

The University of Tokyo, Japan

Toshiji Kanaya

Kyoto University, Japan

Yuji Kawabata

Kyoto University, Japan

Hideaki Kitazawa

National Institute for Materials
Science, Japan

Yoshiaki Kiyanagi

Nagoya University, Japan

Takashi Sakuma

Ibaraki University, Japan

Hirohiko M. Shimizu

Nagoya University, Japan

Jun-ichi Suzuki

Comprehensive Research
Organization for Science andSociety, Japan

Yo Tomota

Ibaraki University, Japan

Masaki Fujita

Tohoku University, Japan

Takatsugu Masuda

The University of Tokyo, Japan
Term: through March 31, 2017164

MLF Annual Report 2014

MLF Operations in 2014

Neutron Advisory Committee (NAC)
NAC-2015 convened 9-10 February, 2015 at the IBARAKI Quantum Beam Research Center, TokaiGroup photo of NAC-2015
Robert McGreevy (chair)
Dimitri Argyriou
Bertrand BlauJohn D Galambos
Toshiji Kanaya
Yoshiaki Kiyanagi
Chang Hee Lee
Dan Alan Neumann
Jamie Schulz
Mitsuhiro Shibayama

Neutron Advisory Committee (9-10 Feb. 2015)
Rutherford Appleton Laboratory
European Spallation Source
Paul Scherrer Institute
Oak Ridge National Laboratory
Kyoto University
Nagoya University
Korea Atomic Energy Research InstituteNational Institute of Standards and Technology
Australian Nuclear Science and Technology Organization
The University of Tokyo

Muon Advisory Committee (MAC)
MAC-2014 convened 11-12 February, 2015 at the KEK Tokai Campus, Tokai

Muon Advisory Committee (11-12 Feb. 2015)
Elvezio Morenzoni (Chair)Toshiyuki Azuma
Klaus Jungmann
Kenya Kubo
Yasuo Nozue
Francis Pratt
Jeff Sonier
Jun Sugiyama

Paul Scherrer Institute
RIKEN
University of Groningen
International Christian University
Osaka University
ISIS
Simon Fraser University
Toyota Central R & D Labs. Inc.

165

MLF Operations in 2014

MLF Annual Report 2014

Workshops, Conferences, Seminars and Schools in 2014
With the increasing level of science activity at the facility, the number and scope of research workshop held under
the auspices of the MLF rapidly expanded in 2014.

International Symposiums held jointly by J-PARC
MLF and CROSS-Tokai

The 14th Korea-Japan Meeting on Neutron Science
7-9 Jan. 2015, IBARAKI Quantum Beam Research Center, Ibaraki
Group Photo of The 14th Korea-Japan
Meeting on Neutron Sciencend

The 2 International Symposium on Science at J-PARC
12-15 Jul. 2014, Tsukuba International Congress Center, Ibaraki

Group Photo of The 2nd International
Symposium on Science at J-PARC

New Opportunities for Better User Group Software
2014 (NOBUGS 2014)24-26 Sep. 2014, KEK Tsukuba campus, Ibaraki
Group Photo of The 10th NOBUGS

Conferences held jointly by J-PARC MLF andCROSS-Tokai
The 3rd IMSS Science Festa, The 6th MLF symposium
and The 32th PF symposium
17-18 Mar. 2015, Tsukuba International Congress Center, Ibaraki

Group Photo of The 3rd IMSS Science Festa

International Collaboration on Advanced Neutron
Sources XXI (ICANS XXI)

Workshops held by KEK

29 Sep. - 3 Oct. 2014, Ibaraki Prefectural Culture Center, Ibaraki

5th Progress report meeting of J-PARC MUSE
26 May 2014, KEK Tokai campus, Ibaraki

Workshop for neutron reflectometry
20 Oct. 2014, KCD Hall, Tokyo
Group Photo of ICANS XXIWorkshop for neutron reflectometry (BL16)
10-11 Nov. 2014, Research Center for Nuclear Physics, Osaka
University, Osaka

166

MLF Annual Report 2014

Workshop for neutron total scattering (BL21)
26 Nov. 2014, KEK Tsukuba campus, Ibaraki

Workshop for neutron spin echo (BL06)

MLF Operations in 2014

The 13th CROSSroads of Users and J-PARC “Physics ofthe strongly correlated electron systems”
2-3 Dec. 2014, IBARAKI Quantum Beam Research Center,
Ibaraki

27 Nov. 2014, KEK Tokai campus, Ibaraki

Workshop for neutron inelastic scattering (BL12)27 Nov. 2014, KEK Tokai campus, Ibaraki

Workshop for polarized neutron scattering (BL23)
18 Dec. 2014, KEK Tsukuba campus, Ibaraki

Workshop for neutron diffraction (BL08, 09)
5 Jan. 2015, KEK Tsukuba campus, Ibaraki

Workshops held by CROSS-Tokai
The 11th CROSSroads of Users and J-PARC “Functional
Interfaces and Reactive Surfaces II”
18-19 Aug. 2014, IBARAKI Quantum Beam Research Center,

Group Photo of The 13nd CROSSroadsof Users and J-PARC

The 14th CROSSroads of Users and J-PARC “Spin liquids
and frustration”
3-4 Feb. 2015, IBARAKI Quantum Beam Research Center,
IbarakiPhoto of The 14th CROSSroadsof Users and J-PARC

IbarakiGroup Photo of The 11th CROSSroadsof Users and J-PARC

The 12th CROSSroads of Users and J-PARC “Characterizing
the structure and functionality of inhomogeneousmaterials using quantum beams”

Workshops and Seminars held by CROSS-Tokaiand other organizations
2014 Workshop on Materials Science
29 Jul. 2014 Essam Kanda Hall, Tokyo

16-17 Sep. 2014, IBARAKI Quantum Beam Research Center,1st 2014 Workshop on Structural Biology

IbarakiPhoto of The 12nd CROSSroadsof Users and J-PARC

3 Oct. 2014, Essam Kanda Hall, Tokyo

2014 Workshop on Metallographic Structure
8 Oct. 2014, KENKYUSHA EIGO Center, Tokyo

2013 The CROSS Trial Use and Ibaraki Beam Line Users
Meeting
22 Oct. 2014, Kagaku-kaikan Hall, Tokyo

Ibaraki Society for Promotion of Use of Neutrons 2014
Meeting of Magnetic Materials
23 Oct. 2014 Essam Kanda Hall, Tokyo167

MLF Operations in 2014

MLF Annual Report 2014

1st 2014 Workshop on Residual Stress and Strain

Schools in 2014

28 Oct. 2014, KENKYUSHA EIGO Center, Tokyo

MLF School 20142014 Workshop on Surfaces and Interfaces

16-19 Dec. 2014, IBARAKI Quantum Beam Research Center,6 Nov. 2014, KENKYUSHA EIGO Center, Tokyo

Ibaraki2014 Workshop on Non-destructive Visualization andAnalysis Methods
25 Nov. 2014, Osaka Science & Technology Center, Osaka

2013 Workshop on Battery Materials
2 Dec. 2014, Essam Kanda Hall, Tokyo

2013 Workshop on Neutron Science 2014
3 Dec. 2014, KENKYUSHA EIGO Center, TokyoJapanese Society for Neutron Science 2014

The 8th KEK Summer Challenge

11-12 Dec. 2014, HOKKAIDO Citizens Actives Center, Hokkaido

19-27 Aug. 2014, KEK Tsukuba Campus, Ibaraki

2014 Workshop on Magnetic Materials
25 Dec. 2014, KENKYUSHA EIGO Center, Tokyo

2013 Workshop on Organic and Polymeric Materials
Neutron Structure Elucidation
5 Feb. 2015, KENKYUSHA EIGO Center, Tokyo

Seminar about the Industrial Application by theComplementarity Use of Synchrotron Radiation and
the Neutron in Hakata
20 Feb. 2015, TKP Conference City, Hakata

Workshop on Computational Science
21 Feb. 2015, Osaka University Nakanoshima Center, Osaka

6th Workshop on Analytical Methods in Small Angle
Scattering
2 Mar. 2015, Tokyo Office of Kyoto University, Tokyo

2nd 2014 Workshop on Residual Stress and Strain
5 Mar. 2015, Essam Kanda Hall, Tokyo

2014 Workshop on Soft Matter Neutron Scattering
12 Mar. 2015, KENKYUSHA EIGO Center, Tokyo

2nd 2014 Workshop on Structural Biology
26 Mar. 2015, KENKYUSHA EIGO Center, Tokyo

Z-Code Training Course
30-31 Mar. 2015, LMJ Tokyo, Tokyo

168

Group Photo of MLF School 2014

Group Photo of the 8th
KEK Summer Challenge
Credit : KEK

MLF Annual Report 2014

MLF Operations in 2014

Award List
The Commendation for Science and Technology by
the Minister of Education, Culture, Sports, Scienceand Technology (MEXT), The Young Scientists’ Prize
Research on Hydrogen Bonds and the Isotope Effect inMinerals in the Earth’s Deep Interior
Asami Sano (JAEA), April 2014th

13 International Conference on Muon Spin
Rotation, Relaxation and Resonance, Best PosterAward
Anomalous 63Cu Knight shift in thiospinel CuIr2S4
Ichihiro Yamauchi(JAEA), June 2014
63rd Annual Denver X-ray Conference, Best XRF
Poster Award
X-ray Fluorescence Imaging of Growing Chemical Patterns
Kenji Sakurai (NIMS) and Tazuko Mizusawa (CROSS), July2014
NOBUGS Poster Award
Visualization and Data Processing Software for SENJU Time-of-Flight Single Crystal Neutron Diffractometer at
J-PARC
Takayasu Hanashima (CROSS), September 2014

JAEA President’s Awards 2014
Inelastic Scattering Study of Material by Complementary
Use of Quantum Beams
Kenji Ishii (JAEA) and Ryoichi Kajimoto (JAEA), October
2014
The JSNS Encouragement Prizes
Development of Horizontal Type Neutron Reflectometer
SOFIA in J-PARC
Norifumi Yamada (KEK), December 2014
The JSNS Encouragement Prizes
Dynamics and Hydration of Bio-molecules Studied by
Neutron Incoherent Scattering and Molecular Simulation
Hiroshi Nakagawa (JAEA), December 2014
JSME Medal for New Technology
Development of Techniques Using Microbubbles to Curb
Pressure Waves in Liquid Metal in order to Realize a HighIntensity Pulsed Neutron Source
Futagawa Masatoshi, Katsuhiro Haga, Hiroyuki Kogawa,Takashi Wakui and Takashi Naoe (JAEA), March 2015

JAEA President’s Awards 2014
Developments of Pressure Wave Mitigation and In-situ
Damage Diagnostic Techniques for the World Most
Powerful Pulsed Spallation Neutron Source
Masatoshi Futagawa, Katsuhiro Haga, Hiroyuki Kogawa,Takashi Wakui, Takashi Naoe, Makoto Teshigawara,
Hidetaka Kinoshita, Masahide Harada, Shin-ichiro
Meigo, Motoki Ooi, Shinichi Sakamoto(JAEA) andHiroshi Fujimori(KEK), October 2014169

MLF operations in 2014

MLF Annual Report 2014

MLF Publication 2014
1

2

3

4

5

K. Munakata, A. Nakao, T. Osakabe, R. Kiyanagi, K. Kaneko, T.
Ohhara, T. Hanashima, K. Oikawa, I. Tamura, T. Kawasaki, K.
Komatsu, and Y. Uwatoko
High-pressure environments of single crystal neutron diffractometer
SENJU/J-PARC
Acta Crystallographica A70 C273 (2014)
A. Nakao, R. Kumai, S. Horiuchi, Y. Tokura, T. Ohhara, T. Hanashima,
K. Munakata, R. Kiyanagi, T. Kawasaki, K. Oikawa, K. Kaneko, and I.
MamuraStructural Study of Ferroelectric Phase in Acid-Base Supramolecule
Acta Crystallographica A70 C553 (2014)
Y. Noda, R. Kiyanagi, T. Ohhara, T. Kawasaki, K. Oikawa, K. Kaneko,
I. Tamura, T. Hanashima, T. Moyoshi, A. Nakao, K. Munakata, and T.
KurodaPrecision of the single crystal neutron diffractometer SENJU at
J-PARC
Acta Crystallographica A70 C400 (2014)
T. Ohhara, R. Kiyanagi, K. Kaneko, T. Kawasaki, K. Oikawa, I.
Tamura, A. Nakao, T. Hanashima, K. Munakata, T. Moyoshi, T.
Kuroda, Y. Yamauchi, and S. Kawamura
SENJU, Extreme Environment Single Crystal Neutron Diffractometer
at J-PARC
Acta Crystallographica A70 C163 (2014)

6

S. Ohisa, G. Matsuba, N. L. Yamada, Y.-J. Pu, H. Sasabe, and J. Kido
Precise Evaluation of Angstrom-Ordered Mixed Interfaces in
Solution-Processed OLEDs by Neutron Reflectometry
Advanced Materials Interfaces 1 9 1400097 (2014)

7

Z. H. Xiong, M. Futakawa, T. Naoe, and K. Maekawa
Very High Cycle Fatigue in Pulsed High Power Spallation Neutron
SourceAdvanced Materials Research 891 536-541 (2014)

8

H. Tatsumoto, Y. Shirai, M. Shiotsu, K. Hata, Y. Naruo, H. Kobayasi,
and Y. Inatani
Forced convection heat transfer of saturated liquid hydrogen invertically-mounted heated pipes
AIP Conference Proceedings 1573 44-51 (2014)

9

H. Tatsumoto, K. Ohtsu, T. Aso, Y. Kawakami, and M. Teshigawara
Operational characteristics of the J-PARC cryogenic hydrogensystem for a spallation neutron source
AIP Conference Proceedings 1573 66-73 (2014)10

T. Ishii, H. Kojitani, S. Tsukamoto, K. Fujino, D. Mori, Y. Inaguma,
N. Tsujino, T. Yoshino, D. Yamazaki, Y. Higo, K. Funakoshi, and M.
AkaogiHigh-Pressure Phase Transitions in FeCr2O4 and Structure Analysis of
New Post-Spinel FeCr2O4 and Fe2Cr2O5 Phases with Meteoritical andPetrological Implications
American Mineralogist 99 1788-1797 (2014)

11

170

R. Kiyanagi, Y. Matsuo, Y. Ishikawa, Y. Noda, T. Ohhara, T. Kawasaki,
K. Oikawa, K. Kaneko, I. Tamura, T. Hanashima, K. Munakata, A.
Nakao, and Y. Kawakita
Proton conduc tion mechanism and phase transition of(Rb,K)3H(SeO4)2
Acta Crystallographica A70 C1359 (2014)

Y. Toh, M. Ebihara, A. Kimura, S. Nakamura, H. Harada, K. Y. Hara, M.
Koizumi, F. Kitatani, and K. Furutaka
Synergistic Effect of Combining Two Nondestructive Analytical

Methods for Multielemental Analysis
Analytical Chemistry 86 24 12030-12036 (2014)12

M. Futakawa
Proton Bombardment in Mercury Target for Neutron Production- Impact dynamics on interface between liquid and solid metals Applied Mechanics and Materials 566 26-33 (2014)

13

T. Naoe, and M. Futakawa
Dynamic Behavior of Liquid Mercury Droplets Colliding with a Solid
Surface
Applied Mechanics and Materials 566 391-396 (2014)

14

T. Wan, T. Naoe, T. Wakui, M. Futakawa, and K. Maekawa
Damage Evaluation by Impulsive Response in Structure Filled with
LiquidApplied Mechanics and Materials 566 629-636 (2014)15

T. Yamaguchi, T. Fukuda, T. Kakeshita, S. Harjo, and T. Nakamoto
Neutron diffraction study on very high elastic strain of 6% in an
Fe3Pt under compressive stress
Applied Physics Letters 104 23 231908 (2014)16

Y. Fujii
An Overview of the Neutron Facilities and the Neutron Scattering
Community in the Asia-Oceania Region
Association of Asia Pacific Physical Societies 24 2 3-6 (2014)

17

K. Akutsu and T. Ohhara
Application and outlook of the pulsed neutron beam at J-PARC,
1; Introduction of neutron beam and neutron crystallography at
J-PARCBUNSEKI 2014 11 617-621 (2014)18

Y. Sakaguchi, H. Asaoka, Y. Uozumi, Y. Kawakita, T. Ito, M. Kubota, D.
Yamazaki, K. Soyama, M. Ailavajhala, M. R. Latif, and M. Mitkova
Studies of Silver Photodiffusion Dynamics in Ag/GexS1–x (x = 0.2 and0.4) Films Using Neutron Reflectometry
Canadian Journal of Physics 92 654-658 (2014)

19

J. Yoshida, A. Ueda, A. Nakao, R. Kumai, H. Nakao, Y. Murakami,
and H. Mori
Solid-Solid Phase Interconversion in an Organic Conductor
Crystal: Hydrogen-Bond-Mediated Dynamic Changes in P-Stacked
Molecular Arrangement and Physical Properties
Chemical Communications 50 15557-15560 (2014)

20

S. C. Lee, A. Ueda, A. Nakao, R. Kumai, H. Nakao, Y. Murakami, and
H. MoriProtonation of Pyridyl-Substituted TTF Derivatives: Substituent
Effects in Solution and in the Proton–Electron Correlated ChargeTransfer Complexes
Chemistry - A European Journal 20 7 1909-1917 (2014)

21

K. Fujii, Y. Esaki, K. Omoto, M. Yashima, A. Hoshikawa, T. Ishigaki,
and J. R. Hester
New Perovskite-Related Structure Family of Oxide-Ion Conducting
Materials NdBaInO4
Chemistry of Materials 26 8 2488-2491 (2014)22

I. Qasim, P. E. R. Blanchard, B. J. Kennedy, C. D. Ling, L.-Y. Jang, T.
Kamiyama, P. Miao, and S. Torii
Soft ferromagnetism in mixed valence Sr1–xLaxTi0.5Mn0.5O3 perovskites
Dalton Transactions 43 18 6909-6918 (2014)

23

M. Futakawa, T. Naoe, H. Kogawa, K. Haga, and K. Okita

MLF Annual Report 2014

Cavitation erosion induced by proton beam bombarding mercury
target for high-power spallation neutron sources
Experimental Thermal and Fluid Science 57 365-370 (2014)
24

25

26

27

A. M. Dymshits, K. D. Litasov, I. S. Sharygin, A. Shatskiy, E. Ohtani, A.
Suzuki, and K. Funakoshi
Thermal Equation of State of Majoritic Knorringite and Its
Significance for Continental Upper Mantle
Featured in Journal of Geophysical Research: Solid Earth 119
8034-8046 (2014)
N. Purevjav, T. Okuchi, N. Tomioka, J. Abe, and S. Harjo
Hydrogen site analysis of hydrous ringwoodite in mantle transitionzone by pulsed neutron diffraction
Geophysical Research Letters 41 19 6718-6724 (2014)
Y. Fujii and T. Kamiyama
Evolution of Neutron Crystallography in Japan
Hamon 24 2 132-140 (2014)
S. Iimura
Switching of Intra-orbital Spin Excitations in Electron-doped Iron
Pnictide Superconductors
Hamon 24 2 121-125 (2014)

MLF operations in 2014

Study on Thermo-mechanically Controlled Processing of Steel using
Neutron Diffraction
Hamon 24 1 40-44 (2014)37

N. Yamada, M. Takeda, and D. Yamazaki
Neutron Reflectometers in J-PARC
Hamon 24 4 288-295 (2014)

38

W. YunA Study on Phase Stress of Centrifugally Cast Duplex Stainless Steelby Neutron Diffraction
Hamon 24 1 28-33 (2014)

39

K. Komatsu, S. Klotz, A. Shinozaki, R. Iizuka, L. E. Bove, and H. Kagi
Performance of ceramic anvils for high pressure neutron scattering
High Pressure Research 34 4 494-499 (2014)

40

T. Okuchi, N. Tomioka, N. Purevjav, J. Abe, S. Harjo, and W. Gong
Structure refinement of sub-cubic-mm volume sample at highpressures by pulsed neutron powder diffraction: application tobrucite in an opposed anvil cellHigh Pressure Research 34 2 273-280 (2014)41

Y. Su, Y. Tomota, S. Harjo, J. Suzuki, and Y. Adachi
In Situ Observations of Microstructural Evolution During Annealingor Deformation in an Electro-Deposited Fine-Grained Iron
In-situ Studies with Photons, Neutrons and Electrons Scattering
II 131-153 (2014)

42

J. Kim, A. Fujiwara, T. Sawada, Y. Kim, K. Sugimoto, K. Kato, H.
Tanaka, M. Ishikado, S. Shamoto, and M. Takata
Evidence of Elec tronic Polarization of the As Ion in the
Superconducting Phase of F-Doped LaFeAsO
International Union of Crystallography Journal 1 155-159 (2014)

28

T. Kume, S. Yamada, and M. Onoo
Structural Change of Human Stratum Corneum by the Treatment ofSurfactant Solutions Studied using Neutron Scattering
Hamon 24 1 15-19 (2014)

29

K. Nakajima, S. Kawamura, and M. Nakamura
Development of 3He Neutron Spin Filter for the Application at an
Intense Pulsed Neutron Source Facility
Hamon 24 2 115-120 (2014)30

H. Nozaki
Ion Conducting Behavior in Secondary Battery Materials Detectedby Quasi-elastic Neutron Scattering Measurements
Hamon 24 1 1 6-10 (2014)

43

M. Futakawa
Material issues relating to high power spallation neutron sources
IOP Conf. Series: Materials Science and Engineering 74 012011(2015)

31

T. Oku, H. Kira, H. Hayashida, K. Sakai, K. Hiroi, T. Shinohara, T.
Ino, M. Ohkawara, K. Ohoyama, S. Takata, K. Ohishi, H. Iwase, N.
Miyata, K. Akutsu, Y. Sakaguchi, M. Takeda, J. Suzuki, K. Aizawa, M.
Arai, and K. Kakurai
Development of ³He Neutron Spin Filter for the Application at an
Intense Pulsed Neutron Source Facility
Hamon 24 4 250-257 (2014)44

H. Terasaki, Y. Shibazaki, K. Nishida, R. Tateyama, S. Takahashi, M.
Ishii, Y. Shimoyama, E. Ohtani, K. Funakoshi, and Y. Higo
Repulsive Nature for Hydrogen Incorporation to Fe3C up to 14 GPa
ISIJ International 54 2637-2642 (2014)

45

K. Ishii and M. Fujita
Observation of electron dynamics by use of three kinds of quantum
beams
Isotope News 728 10-13 (2014)46

T. KaiRecent progress of resonance neutron imaging
Isotope News 727 16-19 (2014)

47

T. Hemmi
Investigation of Strain Using Neutron Diffraction —A Foundation
for Improvement of ITER Conductor Performance
JAEA R&D Review 2014 111 (2014)

48

T. Sato, K. Tomiyasu, K. Ikeda, T. Otomo, M. Feygenson, J.
Neuefeind, K. Yamada, and S.-i. Orimo
Local atomic structural investigations of precursory phenomenon of
the hydrogen release from LiAlD4
Journal of Alloys and Compounds 586 244-247 (2014)

49

K. Ono, N. Inami, K. Saito, Y. Takeichi, M. Yano, T. Shoji, A. Manabe,
A. Kato, Y. Kaneko, D. Kawana, T. Yokoo, and S. Itoh
Observation of spin-wave dispersion in Nd-Fe-B magnets using
neutron Brillouin scattering
Journal of Applied Physics 115 17 17A714(3) (2014)

50

Y. Yasui, Y. Kawamura, Y. Kobayashi, and M. Sato

32

33

34

35

36

Y. Sakaguchi
SKIN2014 Studying Kinetics with Neutrons (SANS and Reflectometry)
Hamon 24 3 215 (2014)
T. Shinohara
Development of the Magnetic Field Imaging using Polarized Pulsed
Neutrons
Hamon 24 2 100-105 (2014)
H. Sueyoshi, N. Ishikawa, K. Yamada, K. Sato, T. Nakagaito, H.
Matsuda, Y. Arakaki, and Y. Tomota
Steel Research using Neutron Beam Techniques / ~In-situ Neutron
Diffraction, Small-angle Neutron Scattering and Residual Stress
Analysis~Hamon 24 1 34-39 (2014)
S.-i. Takata, J.-i. Suzuki, K. Ohishi, H. Iwase, T. Shinohara, T. Oku, T.
Tominaga, Y. Inamura, T. Ito, T. Nakatani, K. Suzuya, K. Aizawa, T.
Otomo, M. Sugiyama, and M. Arai
The Small and Wide Angle Neutron Scattering Instrument TAIKAN at
J-PARC
Hamon 24 4 281-287 (2014)
Y. Tomota

171

MLF operations in 2014

MLF Annual Report 2014

Magnetic and dielectric properties of one-dimensional array of
S = 1/2 linear trimer system Na2Cu3Ge4O12
Journal of Applied Physics 115 17 E125 (2014)
51

52

53

54

55

56

57

T. Naoe, M. Futakawa, R. G. Kenny, and M. Otsuki
Experimental and numerical investigations of liquid mercury droplet
impacts
Journal of Fluid Science and Technology 9 1 JFST0002-1-12 (2014)
T. Mizumoto, D. Tomono, A. Takada, T. Tanimori, S. Komura, H.
Kubo, Y. Matsuoka, Y. Mizumura, K. Nakamura, S. Nakamura, M.
Oda, J. D. Parker, T. Sawano, N. Bando, and A. Nabetani
A Performance Study of an Electron-Tracking Compton Camera witha Compact System for Environmental Gamma-ray Observation
Journal of Instrumentation 10 C06003 (2014)
Y. Mizumura, T. Tanimori, H. Kubo, A. Takada, J. D. Parker, T.
Mizumoto, S. Sonoda, D. Tomono, T. Sawano, K. Nakamura, Y.
Matsuoka, S. Komura, S. Nakamura, M. Oda, K. Miuchi, S. Kabuki, Y.
Kishimoto, S. Kurosawa, and S. Iwaki
Development of a 30 cm-cube Electron-Tracking Compton Camera
for the SMILE-II Experiment
Journal of Instrumentation 8 C05045 (2014)
T. Nakamura, K. Toh, K. Honda, K. Sakasai, K. Soyama, and M.
Katagiri
An empirical formula for calculating the spatial resolution ofa wavelength-shifting fibre detector coupled with a ZnS/ 6LiF
scintillator for detecting thermal neutrons
Journal of Instrumentation 9 11 C11020 (2014)
K. Toh, T. Nakamura, K. Sakasai, K. Soyama, and H. Yamagishi
Evaluation of two-dimensional multiwire neutron detector withindividual line readout under pulsed neutron irradiation
Journal of Instrumentation 9 11 C11019 (2014)
S. Makimura, N. Kawamura, K. M. Kojima, A. Koda, N. Kurosawa, R.
Shimizu, P. Strasser, J. Nakamura, and Y. Miyake
Remote-controlled non-destructive measurement for thermal
conductivity of highly radioactive isotropic graphite used as themuon production target at J-PARC/MUSE
Journal of Nuclear Materials 450 1–3 110-116 (2014)

58

S.-i. Meigo
Conceptual design of proton beam transport system for ADS
facilities at J-PARC
Journal of Nuclear Materials 450 1–3 8-15 (2014)59

S.-i. Meigo, M. Ooi, M. Harada, H. Kinoshita, and A. Akutsu
Radiation damage and lifetime estimation of the proton beam
window at the Japan Spallation Neutron Source
Journal of Nuclear Materials 450 1–3 141-146 (2014)

60

61

62

172

W. Chuajiw, K. Takatori, T. Igarashi, H. Hara, and Y. Fukushima
The influence of aliphatic amines, diamines, and amino acids on thepolymorph of calcium carbonate precipitated by the introduction ofcarbon dioxide gas into calcium hydroxide aqueous suspensions
Journal of Crystal Growth 386 119-127 (2014)

T. Naoe, M. Teshigawara, T. Wakui, H. Kinoshita, H. Kogawa, K.
Haga, and M. Futakawa
Damage inspection of the first mercury target vessel of JSNS
Journal of Nuclear Materials 450 1–3 123-129 (2014)
M. Ooi, M. Teshigawara, M. Harada, T. Naoe, F. Maekawa, and Y.
Kasugai
Development of Au–In–Cd decoupler by a hot isostatic pressing (HIP)
technique for short pulsed spallation neutron source
Journal of Nuclear Materials 450 1–3 117-122 (2014)
B. W. Riemer, M. W. Wendel, D. K. Felde, R. L. Sangrey, A. Abdou,
D. L. West, T. J. Shea, S. Hasegawa, H. Kogawa, T. Naoe, C. H. Farny,

and A. L. Kaminsky
Small gas bubble experiment for mitigation of cavitation damage
and pressure waves in short-pulse mercury spallation targets
Journal of Nuclear Materials 450 1–3 192-203 (2014)
63

J. D. Parker, M. Harada, K. Hattori, S. Iwaki, S. Kabuki, Y. Kishimoto,H. Kubo, S. Kurosawa, Y. Matsuoka, K. Miuchi, T. Mizumoto, H.
Nishimura, T. Oku, T. Sawano, T. Shinohara, J. Suzuki, A. Takada, T.
Tanimori, K. Ueno, M. Ikeno, M. Tanaka, and T. Uchida
Applications of a Micro-Pixel Chamber (μPIC) Based, Time-Resolved
Neutron Imaging Detector at Pulsed Neutron Beams
Journal of Physics: Conference Series 502 012048 (2014)64

H. Hayashida, K. Soyama, D. Yamazaki, R. Maruyama, and K.
Yamamura
Development and demonstration of a multi-channel spheroidal
focusing device for neutron beams
Journal of Physics: Conference Series 528 1 12007 (2014)

65

H. Hayashida, T. Oku, H. Kira, K. Sakai, M. Takeda, Y. Sakaguchi, T.
Ino, T. Shinohara, K. Ohoyama, J. Suzuki, K. Kakurai, M. Mizusawa,
N. Miyata, D. Yamazaki, R. Maruyama, K. Soyama, and M. Arai
Development and Demonstration of In-situ SEOP 3He Spin Filter
System for Neutron Spin Analyzer on the SHARAKU Polarized
Neutron Reflectometer at J-PARC
Journal of Physics: Conference Series 528 1 012020 (2014)

66

S. Hosokawa, J. F. Bérar, N. Boudet, S. Kohara, J. Stellhorn, W. C.
Pilgrim, A. Zeidler, H. Kato, Y. Kawakita, and T. Otomo
A combination of anomalous x-ray scattering and neutron
diffraction for structural characterizations of Zr63 Ni25 Al12 metallic
glass
Journal of Physics: Conference Series 502 1 12023 (2014)

67

T. Ino, H. Otono, K. Mishima, and T. Yamada
Precision neutron flux measurement with a neutron beam monitor
Journal of Physics: Conference Series 528 1 12039 (2014)

68

S. Itoh, T. Yokoo, D. Kawana, Y. Kaneko, Y. Tokura, M. Fujita, K.
Yoshida, K. Saito, N. Inami, Y. Takeichi, K. Ono, and Y. Endoh
Neutron Brillouin Scattering Experiments with Pulsed Neutrons on
High Resolution Chopper Spectrometer HRC
Journal of Physics: Conference Series 502 1 12043 (2014)

69

S. Itoh, S. Yano, T. Yokoo, S. Satoh, D. Kawana, Y. Kousaka, J.
Akimitsu, and Y. Endoh
Spin Waves in Ferromagnetic Phase of MnPJournal of Physics: Conference Series 502 1 12044 (2014)70

R. Kajimoto, M. Fujita, K. Nakajima, K. Ikeuchi, Y. Inamura, M.
Nakamura, and T. Imasato
Inelastic neutron scattering study of phonon anomalies in
La1.5Sr0.5NiO4Journal of Physics: Conference Series 502 1 12056 (2014)

71

N. Kawamura, A. Toyoda, M. Aoki, K. Shimomura, T. Mibe, Y.
Nakatsugawa, M. Otani, N. Saito, and Y. Miyake
H line; a beam line for fundamental physics study
Journal of Physics: Conference Series 551 1 012062 (1-6) (2014)72

Y. Kobayashi, S. Kototani, M. Itoh, and M. Sato
Emergence of Superconducting and/or Magnetic Ordering Tuned by
Fe-Vacancy Order in Alkali Metal Intercalated Fe Chalcogenides
Journal of Physics: Conference Series 568 022024 (2014)

73

K. M. Kojima, T. Murakami, Y. Takahashi, H. Lee, S. Y. Suzuki, A.
Koda, I. Yamauchi, M. Miyazaki, M. Hiraishi, H. Okabe, S. Takeshita,
R. Kadono, T. U. Ito, W. Higemoto, S. Kanda, Y. Fukao, N. Saito, M.
Saito, M. Ikeno, T. Uchida, and M. M. Tanaka
New μSR spectrometer at J-PARC MUSE based on Kalliope detectors
Journal of Physics: Conference Series 551 1 012063 (1-6) (2014)

MLF Annual Report 2014

74

R. M. Macrae, C. Upchurch, D. K. Rose, Y. Miyake, A. Koda, J. S.
Lord, and P. S. Shuttleworth
Paramagnetic muon states in mesoporous carbon materials
Journal of Physics: Conference Series 551 1 012040 (1-7) (2014)

75

T. Masui, H. Kishimoto, T. Kikuchi, S. Ohira-Kawamura, Y. Inamura,
T. Koga, and K. Nakajima
Quasielastic Neutron Scattering Study on Polymer Nanocomposites
Journal of Physics: Conference Series 502 1 12057 (2014)

76

77

78

P. Miao, S. Torii, M. Yonemura, Y. Ishikawa, J. Zhang, and T.
Kamiyama
Structure analysis on small molecular crystal by high resolution
neutron powder diffraction
Journal of Physics: Conference Series 502 1 12055 (2014)
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
Production of ultra cold neutrons by a doppler shifter with pulsed
neutrons at J-PARC
Journal of Physics: Conference Series 528 1 12030 (2014)
Y. Miyake, K. Shimomura, N. Kawamura, P. Strasser, A. Koda,
H. Fujimori, Y. Ikedo, S. Makimura, Y. Kobayashi, J. Nakamura,
K. M. Kojima, T. Adachi, R. Kadono, S. Takeshita, K. Nishiyama, W.
Higemoto, T. Ito, K. Nagamine, H. Ohata, Y. Makida, M. Yoshida, T.
Okamura, R. Okada, and T. Ogitsu
Current status of the J-PARC muon facility, MUSE
Journal of Physics: Conference Series 551 1 012061 (1-7) (2014)

79

M. Miyazaki, R. Kadono, M. Hiraishi, I. Yamauchi, A. Koda, K. M.
Kojima, I. Kawasaki, I. Watanabe, Y. Okamoto, and Z. Hiroi
Spin dynamics of Mn pyrochlore lattice in YMn2 Zn20–xInx
cJournal of Physics: Conference Series 551 1 012019 (1-6) (2014)

80

T. Nakamura, K. Toh, K. Honda, A. Birumachi, M. Ebine, K. Sakasai,
K. Soyama, and M. Katagiri
Development of a wavelength-shifting-fibre-based scintillator
neutron detector as an alternative to 3He at J-PARC/MLF
Journal of Physics: Conference Series 528 1 12042 (2014)

81

T. Nakamura, M. Katagiri, N. Tsutsui, K. Toh, N. J. Rhodes, E. M.
Schooneveld, H. Ooguri, Y. Noguchi, K. Sakasai, and K. Soyama
Development of a ZnS/ 10 B 2 O 3 scintillator with low-afterglow
phosphor
Journal of Physics: Conference Series 528 1 12043 (2014)

82

83

84

J. Nakamura, Y. Oishi, N. Saito, K. Miyazaki, K. Okamura, W.
Higemoto, Y. Ikedo, K. M. Kojima, P. Strasser, T. Nagatomo, S.
Makimura, Y. Miyake, N. Kawamura, K. Yokoyama, D. Tomono,
K. Shimomura, S. Wada, A. Koda, Y. Kobayashi, H. Fujimori, R.
Kadono, and K. Nishiyama
Optimal crossed overlap of coherent vacuum ultraviolet radiationand thermal muonium emission for μSR with the Ultra Slow Muon
Journal of Physics: Conference Series 551 1 012066 (1-6) (2014)
J. Nakamura, T. Nagatomo, Y. Oishi, Y. Ikedo, P. Strasser, N. Saito,
K. Miyazaki, K. Yokoyama, K. Okamura, Y. Miyake, S. Makimura, K.
Nishiyama, K. Shimomura, N. Kawamura, A. Koda, W. Higemoto, S.
Wada, M. Iwasaki, and E. Torikai
Ultra Slow Muon Microscope at MUSE / J-PARC
Journal of Physics: Conference Series 502 1 012042 (1-4) (2014)
K. Ohoyama, T. Yokoo, S. Itoh, T. Ino, M. Ohkawara, T. Oku, S.
Tasaki, K. Iwasa, T. J. Sato, S. Ishimoto, K. Taketani, H. Kira, Y.
Sakaguch, M. Nanbu, H. Hiraka, H. M. Shimizu, M. Takeda, M.
Hino, K. Hayashi, M. Kenzelmann, U. Fliges, and P. Hautle
Concepts of Neutron Polarisation Analysis Devices for a New
Neutron Chopper Spectrometer, POLANO, in J-PARC
Journal of Physics: Conference Series 502 1 12051 (2014)

MLF operations in 2014

85

T. Okuda, H. Hata, T. Eto, K. Nishina, H. Kuwahara, M. Nakamura,and R. Kajimoto
Effects of Mn Substitution on the Thermoelectric Properties of theElectron-Doped Perovskite Sr1−xLaxTiO3
Journal of Physics: Conference Series 568 022035 (2014)

86

A. D. Pant, K. Nagamine, I. Shiraki, E. Torikai, K. Shimomura, F. L.
Pratt, H. Ariga, K. Ishida, and J. S. Schultz
Muonium response to oxygen content in biological aqueous
solutions for cancer research
Journal of Physics: Conference Series 551 1 012043 (1-6) (2014)

87

K. Sakai, T. Oku, H. Hayashida, H. Kira, T. Shinohara, K. Oikawa, M.
Harada, K. Kakurai, K. Aizawa, M. Arai, Y. Sakaguchi, J. Suzuki, T.
Ino, and K. Ohoyama
Development of Portable Polarized 3He Spin Flipper for Polarized
Neutron Experiment at J-PARC
Journal of Physics: Conference Series 528 012016 (2014)88

D. Sakurai, J. Chiba, T. Ino, N. Kakusho, N. Kaneko, R. Katayama, M.
Kitaguchi, K. Mishima, S. Muto, K. Ozeki, Y. Seki, H. M. Shimizu, S.
Yamashita, T. Yoshioka, and D. Nishimura
Development of a new neutron mirror made of deuterated
Diamond-like carbon
Journal of Physics: Conference Series 528 1 12010 (2014)89

S. Satoh, N. L. Yamada, and S. Muto
Detector development for a high-flux neutron reflectometer
Journal of Physics: Conference Series 502 1 12050 (2014)90

Y. Shirai, K. Hikawa, M. Shiotsu, H. Tatsumoto, Y. Naruo, H.
Kobayashi, and Y. Inagaki
Cooling Stability Test of MgB2 Wire Immersed in Liquid Hydrogen
under External Magnetic Field
Journal of Physics: Conference Series 507 2 22031 (2014)

91

P. Strasser, Y. Ikedo, S. Makimura, J. Nakamura, K. Nishiyama,
K. Shimomura, H. Fujimori, T. Adachi, A. Koda, N. Kawamura,
Y. Kobayashi, W. Higemoto, T. U. Ito, T. Nagatomo, E. Torikai, R.
Kadono, and Y. Miyake
Design and construction of the ultra-slow muon beamline at
J-PARC/MUSE
Journal of Physics: Conference Series 551 1 012065 (1-7) (2014)92

J. Sugiyama, H. Nozaki, I. Umegaki, M. Harada, Y. Higuchi, E. J.
Ansaldo, J. H. Brewer, Y. Miyake, G. Kobayashi, and R. Kanno
Structural, magnetic, and diffusive nature of olivine-type Nax FePO4
Journal of Physics: Conference Series 551 1 012012 (1-7) (2014)

93

T. Suzuki, I. Watanabe, F. Yamada, Y. Ishii, K. Ohishi, T. Goto, and H.
TanakaGradual Evolution in Spin Dynamics of TlCu1–xMgxCl3 Probed by
Muon-Spin Relaxation (μSR) Technique
Journal of Physics: Conference Series 502 012041 (2014)

94

H. Tatsumoto, Y. Shirai, M. Shiotsu, Y. Naruo, H. Kobayashi, and Y.
Inatani
Development of an experimental system for characterization ofhigh-temperature superconductors cooled by liquid hydrogen underthe external magnetic field
Journal of Physics: Conference Series 507 2 22042 (2014)

95

H. Tatsumoto, Y. Shirai, M. Shiotsu, Y. Naruo, H. Kobayashi, and Y.
Inatani
Forced convection heat transfer from a wire inserted into avertically-mounted pipe to liquid hydrogen flowing upward
Journal of Physics: Conference Series 568 3 32017 (2014)96

K. Toh, T. Nakamura, K. Sakasai, K. Soyama, and H. Yamagishi
Performance evaluation of high-pressure MWPC with individual line
readout under Cf-252 neutron irradiation
Journal of Physics: Conference Series 528 1 12045 (2014)173

MLF operations in 2014

97

98

99

MLF Annual Report 2014

T. Tominaga, S. Takata, J. Suzuki, K. Aizawa, H. Seto, and M. Arai
Adsorption of Water to Double-Network Polymers Having a
Hierarchical Structure
Journal of Physics: Conference Series 502 012058 (2014)
S. Torii, M. Yonemura, Y. Ishikawa, P. Miao, R. Tomiyasu, S. Satoh, Y.
Noda, and T. Kamiyama
Improvement of Instrument Devices for Super High Resolution
Powder Diffractometer at J-PARC
Journal of Physics: Conference Series 502 1 12052 (2014)
M. Toyoda, Y. Kobayashi, M. Itoh, and M. Sato
Lower Symmetrical Behaviour of Electronic State in the FeAs Planeof Ba(Fe1–xCox )2 As2 -75As NMR StudyJournal of Physics: Conference Series 568 022029 (2014)

100 I. Umegaki , H. Nozaki, M. Harada, Y. Higuchi, T. Noritake, M.
Matsumoto, S-i. Towata, E. J. Ansaldo, J. H. Brewer, A. Koda, Y.
Miyake, and J. Sugiyama
In situ μ+SR measurements on the hydrogen desorption reaction ofmagnesium hydride
Journal of Physics: Conference Series 551 1 012036 (1-6) (2014)
101 I. Yamauchi, M. Miyazaki, M. Hiraishi, A. Koda, K. M. Kojima, R.
Kadono, and H. Nakamura
Muon Knight shift in d-electron heavy fermion compoundY0.95Sc0.05Mn2
Journal of Physics: Conference Series 551 1 012002 (1-6) (2014)
102 T. Yokoo, K. Ohoyama, S. Itoh, J. Suzuki, M. Nanbu, N. Kaneko, K.
Iwasa, T. J. Sato, H. Kimura, and M. Ohkawara
Construction of Polarized Inelastic Neutron Spectrometer in J-PARC
Journal of Physics: Conference Series 502 1 12046 (2014)
103 T. Yokoo, S. Itoh, D. Kawana, H. Yoshizawa, and J. Akimitsu
Dynamical properties of spins and holes in carrier doped quantum
Haldane chain
Journal of Physics: Conference Series 502 1 12045 (2014)
104 T. Yokoo, S. Itoh, S. Ibuka, H. Yoshizawa, and J. Akimitsu
Spin and Hole Dynamics in Carrier-Doped Quantum Haldane Chain
Journal of Physics: Conference Series 568 4 42035 (2014)
105 M. Yonemura, M. Hirayama, K. Suzuki, R. Kanno, N. Torikai, and N. L.
YamadaDevelopment of Spectroelectrochemical Cells for in situ Neutron
Reflectometry
Journal of Physics: Conference Series 502 1 12054 (2014)
106 M. Yonemura, K. Mori, T. Kamiyama, T. Fukunaga, S. Torii, M.
Nagao, Y. Ishikawa, Y. Onodera, D. S. Adipranoto, H. Arai, Y.
Uchimoto, and Z. Ogumi
D evelopment of SPICA, New D edicated Neutron Powder
Diffractometer for Battery Studies
Journal of Physics: Conference Series 502 1 12053 (2014)
107 R. Iizuka, K. Komatsu, H. Kagi, T. Nagai, A. Sano-Furukawa, T.
Hattori, H. Gotou, and T. Yagi
Phase transitions and hydrogen bonding in deuterated calcium
hydroxide: High-pressure and high-temperature neutron diffraction
measurements
Journal of Solid State Chemistry 218 95-102 (2014)
108 L. Kuo, H. Yufei, W. Yingxia, K. Takashi, W. Bingwu, L. Zhaofei, and L.
JianhuaSyntheses and proper ties of a family of new compounds
RE3Sb3Co2O14(RE=La, Pr, Nd, Sm–Ho) with an ordered pyrochlore
structure
Journal of Solid State Chemistry 217 80-86 (2014)
109 I. Qasim, P. E. R. Blanchard, B. J. Kennedy, T. Kamiyama, P. Miao,
and S. Torii

174

Structural and electronic properties of Sr1−xCaxTi0.5Mn0.5O3
Journal of Solid State Chemistry 213 293-300 (2014)
110 Y. Kameda, T. Miyazaki, T. Otomo, Y. Amo, and T. Usuki
Neutron Diffraction Study on the Structure of Aqueous LiNO 3
Solutions
Journal of Solution Chemistry 43 9-10 1588-1600 (2014)
111 J. Bang, S. Matsuishi, H. Hiraka, F. Fujisaki, T. Otomo, S. Maki, J.-i.
Yamaura, R. Kumai, Y. Murakami, and H. Hosono
Hydrogen Ordering and New Polymorph of Layered Perovskite
Oxyhydrides: Sr2VO4–xHx
Journal of the American Chemical Society 136 20 7221-7224(2014)
112 A. Ueda, S. Yamada, T. Isono, H. Kamo, A. Nakao, R. Kumai, H.
Nakao, Y. Murakami, K. Yamamoto, Y. Nishio, and H. Mori
Hydrogen-Bond-Dynamics-Based Switching of Conductivity andMagnetism: A Phase Transition Caused by Deuterium and ElectronTransfer in a Hydrogen-Bonded Purely Organic Conductor Crystal
Journal of the American Chemical Society 136 34 12184-12192(2014)
113 Y. Fujii
ཎᏊ⅔୰ᛶᏊ䛾฼⏝Journal of the Crystallographic Society of Japan (2014)
114 T. Ohhara
Recent Advance of the Neutron Crystal Chemistry by using HighIntensity Neutron Beam at J-PARC
Journal of the Crystallographic Society of Japan 56 5 301-306(2014)
115 M. Hiraishi, R. Kadono, M. Miyazaki, I. Yamauchi, A. Koda, K. M.
Kojima, M. Ishikado, S. Wakimoto, and S. Shamoto
Cooperative Order in the Weakly Magnetic Domain of LaFeAsO1−xFx
near the Doping Phase Boundary
Journal of the Physical Society of Japan 83 103707 (1-5) (2014)
116 K. Kamazawa, M. Harada, T. Araki, Y. Matsuo, M. Tyagi, and J.
Sugiyama
Interrelationship between the Number of Mobile Proton, Diffusion
Coefficient and AC Conductivity in Superprotonic Conductors,
CsHSO4 and Rb3H(SeO4)2
Journal of the Physical Society of Japan 83 074604 (2014)
117 Y. Kobayashi, T. Iida, K. Suzuki, T. Kawamata, M. Itoh, and M. Sato75
As NQR and NMR Studies on the Superconducting State of
Ca10Pt4As8(Fe1–xPtxAs)10
Journal of the Physical Society of Japan 83 014712 (2014)
118 K. Motoya, T. Moyoshi, and M. Matsuda
Long-Time Variation in Magnetic Structure of Ce0.98La0.02Ir3Si2: Effectof Randomness on Time Variation
Journal of the Physical Society of Japan 83 2 24708 (2014)
119 H. Shigematsu, K. Nishiyama, Y. Kawamura, and H. Mashiyama
Neutron and X-ray Scattering Studies of Rb2CoCl4 and Successive
Phase Transition in A2BX4-Type Crystals
Journal of the Physical Society of Japan 83 124601 (2014)
120 T. Yamamoto, Y. Nakazawa, M. Tamura, A. Nakao, A. Fukaya, R.
Kato, and K. Yakushi
Property of the Valence-Bond Ordering in Molecular Superconductor
with a Quasi-Triangular Lattice
Journal of the Physical Society of Japan 83 053703 (2014)
121 T. Yamazaki, Y. Tabata, T. Waki, T. J. Sato, M. Matsuura, K. Ohoyama,
M. Yokoyama, and H. Nakamura
Novel Magnetic Chiral Structures and Peculiar Temperature
Hysteresis in the Metallic Helimagnet MnPJournal of the Physical Society of Japan 83 054711 (2014)

MLF Annual Report 2014

122 K. T. Lai, A. Takemori, S. Miyasaka, S. Tajima, A. Nakao, H. Nakao, R.
Kumai, and Y. Murakami
Suppression of Superconductivity around x = 0.5–0.7 in
LaFeP1–x AsxO0.95F0.05
JPS Conference Proceedings 1 012104 (2014)
123 H. Ariga, K. Shimomura, K. Ishida, F. Pratt, K. Yoshizawa, W.
Higemoto, E. Torikai, and K. Asakura
Detection of Oxygen Vacancy in Rutile TiO2 Single Crystal by μSR
Measurement
JPS Conference Proceedings 2 010307 (1-4) (2014)
124 M. Futakawa
Targetry overview - Various target concepts and expectable next
generation targets in power frontier applications JPS Conference Proceedings 8 001002 (1-12) (2015)
125 L. Hao, K. Iwasa, H. Kobayashi, K. Nakajima, S. Ohira-Kawamura, T.
Kikuchi, D. Chen, Y. Liu, Z. Liu, S. Li, and D. Hu
Effects of Co Substitution on the Magnetic Excitation in Heavy
Fermion Compound PrFe4P12
JPS Conference Proceedings 3 11088 (2014)
126 M. Harada, K. Oikawa, M. Ooi, T. Kai, T. Shinohara, K. Sakai, and F.
Maekawa
Performance of Optical Devices for Energy-Selective Neutron
Imaging in NOBORU at J-PARC
JPS Conference Proceedings 1 1 14015 (2014)
127 S. Harjo, J. Abe, K. Aizawa, W. Gong, and T. Iwahashi
Deformation Behavior of An Austenitic Steel by Neutron Diffraction
JPS Conference Proceedings 1 14017 (2014)
128 W. Higemoto, A. Koda, R. Kadono, Y. Yoshida, and Y. Ōnuki
Investigation of Spontaneous Magnetic Field in Spin-Triplet
Superconductor Sr2RuO4
JPS Conference Proceedings 2 010202 (1-5) (2014)
129 K. Iida, K. Ikeuchi, M. Ishikado, J. Suzuki, R. Kajimoto, M.
Nakamura, Y. Inamura, and M. Arai
Energy- and Q-Resolution Investigations of a Chopper Spectrometer
4SEASONS at J-PARC
JPS Conference Proceedings 1 014016 (2014)
130 Y. Ikedo, Y. Miyake, K. Shimomura, P. Strasser, N. Kawamura,
K. Nishiyama, S. Makimura, H. Fujimori, A. Koda, J. Nakamura,
T. Nagatomo, Y. Kobayashi, T. Adachi, A. D. Pant, T. Ogitsu, T.
Nakamoto, K. Sasaki, H. Ohhata, R. Okada, A. Yamamoto, Y.
Makida, M. Yoshida, T. Okamura, R. Ohkubo, W. Higemoto, T. U.
Ito, K. Nakahara, and K. Ishida
U-Line at MLF/J-PARC for Ultra Slow Muon Microscopy
JPS Conference Proceedings 2 010103 (1-4) (2014)
131 K. Ikeuchi, M. Sato, R. Kajimoto, Y. Kobayashi, K. Suzuki, M. Itoh, P.
Bourges, A. D. Christianson, H. Nakamura, and M. MachidaPhonons and Spin Excitations in Fe-Based Superconductor
Ca10Pt4 As8 (Fe1−x Ptx As)10 (x~0.2)
JPS Conference Proceedings 3 015043 (2014)
132 R. Kajimoto, K. Nakajima, S. Ohira-Kawamura, Y. Inamura, T.
Okuda, and K. Tomiyasu
Low-Energy Spin Fluctuations in CuCrO2 and Cu0.85Ag0.15CrO2 Studied
by Inelastic Neutron Scattering
JPS Conference Proceedings 3 14018 (2014)
133 S. Kanda, H. Fujimori, Y. Fukao, Y. Ikedo, K. Ishida, M. Iwasaki, N.
Kawamura, K. M. Kojima, M. Lee, S. Makimura, T. Mibe, Y. Miyake, J.
Nakamura, Y. Nagashima, T. Nagatomo, K. Nagumo, S. Nishimura,
S. Okada, N. Saito, K. Shimomura, T. Suzuki, P. Strasser, K. Ueno,
and E. Won
Development of High-Rate Positron Tracker for the Muonium
Production Experiment at J-PARC

MLF operations in 2014

JPS Conference Proceedings 2 010404 (1-7) (2014)
134 N. Kawamura, A. Toyoda, T. Mibe, N. Saito, M. Aoki, K. Shimomura,and Y. Miyake
H Line; A Beamline for Fundamental Physics in J-PARC
JPS Conference Proceedings 2 010112 (1-6) (2014)
135 T. Kawasaki, K. Kaneko, N. Aso, A. Nakamura, M. Hedo, T. Nakama,
Y. Onuki, T. Ohhara, R. Kiyanagi, K. Oikawa, I. Tamura, A. Nakao, K.
Munakata, and T. Hanashima
Single Crystal Neutron Diffraction Study of High Neutron Absorbing
Compound EuGa4
JPS Conference Proceedings 1 014009 (2014)
136 R. Kiyanagi, Y. Ishikawa, and Y. Noda
Proton Conduction Path in Rb 3 H(S eO 4 ) 2 Studied by High
Temperature Neutron Single Crystal Diffraction
JPS Conference Proceedings 1 12034 (2014)
137 Y. Kousaka, N. Ikeda, T. Ogura, T. Yoshii, J. Akimitsu, K. Ohishi,
J. Suzuki, H. Hiraka, M. Miyagawa, S. Nishihara, K. Inoue, and J.
KishineChiral Magnetic Soliton Lattice in MnSi
JPS Conference Proceedings 2 010205 (2014)
138 S. Makimura, M. Onoi, M. Wakasugi, T. Nagatomo, Y. Ikedo, P.
Strasser, K. Shimomura, J. Nakamura, K. Nishiyama, and Y. Miyake
Development of Manufacturing Method of Highly Pure Tungsten
Foil for Thermal Muonium Generation
JPS Conference Proceedings 2 010104 (1-6) (2014)
139 Y. Miyake, Y. Ikedo, K. Shimomura, P. Strasser, N. Takashi, J.
Nakamura, S. Makimura, N. Kawamura, H. Fujimori, A. Koda, Y.
Kobayashi, K. Nishiyama, R. Kadono, W. Higemoto, T. U. Ito, T.
Ogitsu, Y. Makida, K. Sasaki, T. Adachi, and E. Torikai
Ultra Slow Muon Project at J-PARC MUSEJPS Conference Proceedings 2 010101 (1-6) (2014)
140 K. Nagamine
Past, Present and Future of Ultra-Slow Muons
JPS Conference Proceedings 2 010001 (-8) (2014)
141 T. Nagatomo, Y. Ikedo, P. Strasser, S. Makimura, J. Nakamura, K.
Nishiyama, K. Shimomura, N. Kawamura, A. Koda, H. Fujimori, Y.
Kobayashi, T. U. Ito, W. Higemoto, A. D. Pant, R. Kadono, E. Torikai,
and Y. Miyake
Construction of Ultra Slow Muon Beam Line at J-PARC
JPS Conference Proceedings 2 010102 (1-5) (2014)
142 M. Nakamura and R. Kajimoto
General Formulae for the Optimized Design of Fermi Chopper
Spectrometer
JPS Conference Proceedings 1 014018 (2014)
143 J. Nakamura, Y. Oishi, N. Saito, K. Miyazaki, K. Yokoyama, K.
Okamura, S. Makimura, Y. Miyake, T. Nagatomo, P. Strasser, Y.
Ikedo, D. Tomono, K. Shimomura, S. Wada, N. Kawamura, A. Koda,
and K. Nishiyama
Transport of Coherent VUV Radiation to Muon U-Line for Ultra Slow
Muon Microscope
JPS Conference Proceedings 2 010108 (1-7) (2014)
144 T. Nakatani, Y. Inamura, K Moriyama, T. Ito, S. Muto, and T. Otomo
Event Recording Data Acquisition System and Experiment DataManagement System for Neutron Experiments at MLF, J-PARC
JPS Conference Proceedings 1 014010 (2014)
145 H. Nozaki, S. Ohta, M. Harada, M. Måsson, D. Sheptyakov, V.
Pomjakushin, I. Watanabe, Y. Ikedo, Y. Miyake, and J. Sugiyama
Li-Ion Dynamics in Li5+xLa3ZrxNb2−xO12
JPS Conference Proceedings 2 010303 (1-6) (2014)175

MLF operations in 2014

MLF Annual Report 2014

146 K. Oikawa, T. Kawasaki, T. Ohhara, R. Kiyanagi, K. Kaneko, I.
Tamura, T. Nakamura, M. Harada, A. Nakao, T. Hanashima, K.
Munakata, H. Kimura, Y. Noda, M. Takahashi, and T. Kiyotani
Instrument Design and Performance Evaluation of a New Single
Crystal Neutron Diffractometer SENJU at J-PARC
JPS Conference Proceedings 1 014013 (2014)
147 K. Oikawa, M. Harada, and F. Maekawa
Study on the Pulse Shape of Thermal and Cold Neutrons Provided by
the Decoupled Moderator of JSNSJPS Conference Proceedings 1 1 14012 (2014)
148 M. Sato, K. Ikeuchi, R. Kajimoto, Y. Kobayashi, Y. Yasui, K. Suzuki,
M. Itoh, M. Nakamura, Y. Inamura, M. Arai, P. Bourges, A. D.
Christianson, H. Nakamura, and M. Machida
On the Superconducting Symmetry of Fe-Based Systems -Impurity
Effects and Microscopic Magnetic BehaviorJPS Conference Proceedings 1 014007 (2014)
149 K. Sato, M. Matsuura, M. Fujita, R. Kajimoto, S. Ji, K. Ikeuchi, M.
Nakamura, Y. Inamura, M. Arai, M. Enoki, and K. Yamada
Temperature Dependence of Spin Fluctuations in Underdoped
La1.90Sr0.10CuO4
JPS Conference Proceedings 3 017010 (2014)
150 K. Shimomura, R. Kadono, A. Koda, K. Nishiyama, W. Higemoto,and T. U. Ito
μSR Study on Isolated Hydrogen and Oxygen Vacancy in SrTiO3
JPS Conference Proceedings 2 010308 (1-4) (2014)
151 Y. Sugawara, A. D. Pant, W. Higemoto, K. Shimomura, E. Torikai,
and K. Nagamine
Hydration Effects on Electron Transfer in Biological Systems Studied
by μSRJPS Conference Proceedings 2 010310(1-5) (2014)
152 K. S. Tanaka, M. Aoki, H. Iinuma, Y. Ikedo, K. Ishida, M. Iwasaki,
Y. Ueno, R. Ohkubo, T. Ogitsu, R. Kadono, O. Kamigaito, N.
Kawamura, D. Kawall, S. Kanda, K. Kubo, T. Kume, A. Koda, K.
Kojima, N. Saito, N. Sakamoto, K. Sasaki, K. Shimomura, M.
Sugano, D. Tomono, A. Toyoda, H. A. Torii, E. Torikai, K. Nagamine,
K. Nishiyama, P. Strasser, Y. Fukao, Y. Fujiwara, Y. Matsuda, T. Mibe, Y.
Miyake, and M. Yoshida
Measurement of Muonium Hyperfine Splitting at J-PARC
JPS Conference Proceedings 2 010405 (1-6) (2014)

158 C. M. Phan, C. V. Nguyen, S.-i. Yusa, and N. L. Yamada
Synergistic Adsorption of MIBC/CTAB Mixture at the Air/Water
Interface and Applicability of Gibbs Adsorption Equation
Langmuir 30 20 5790-5796 (2014)
159 H. Komiyama, R. Sakai, S. Hadano, S. Asaoka, K. Kamata, T. Iyoda,
M. Komura, T. Yamada, and H. Yoshida
Enormously Wide Range Cylinder Phase of Liquid Crystalline
PEObPMA(Az) Block Copolymer
Macromolecules 47 5 1777–1782 (2014)
160 J. Abe, K. Sekine, S. Harjo, W. Gong, and K. Aizawa
Strain Analysis in Geological Materials Using Neutron Diffraction
and AE Signal Measurement at J-PARC/BL19" TAKUMI"
Materials Science Forum 777 219-224 (2014)
161 S. Harjo, K. Aizawa, J. Abe, W. Gong, T. Ito, T. Kawasaki, and T.
IwahashiEngineering & Related Studies at J-PARC
Materials Science Forum 777 12-18 (2014)
162 S. Harjo, T. Hemmi, J. Abe, W. Gong, Y. Nunoya, K. Aizawa, T. Ito, N.
Koizumi, S. Machiya, and K. Osamura
Residual Strains in ITER Conductors by Neutron Diffraction
Materials Science Forum 777 84-91 (2014)
163 T. Hirano, K. Hidaka, D. Takamatsu, N. Takahashi, K. Shishido, M.
Sasaki, and Y. Kawashima
Analysis of Residual Stresses in Pistons of Motor Vehicle Engines
Using Neutron Diffraction at J-PARC
Materials Science Forum 772 27-32 (2014)
164 T. Ito, S. Harjo, Y. Inamura, T. Nakatani, T. Kawasaki, J. Abe, and K.
AizawaUtilization of an event-recording system for neutron diffraction
experiments
Materials Science Forum 783-786 2071-2074 (2014)
165 X. Z. Jin, T. Nakamoto, K. Tsuchiya, A. Yamamoto, T. Ogitsu, M.
Sugano, S. Harjo, J. Abe, W. Gong, T. Iwahashi, A. Kikuchi, T.
Takeuchi, Y. Yanagisawa, M. Takahashi, and H. Maeda
Recent R&D on Superconducting Wires for High-Field Magnet
Materials Science Forum 783-786 2081-2090 (2014)

153 T. Tominaga, S.-i. Takata, J.-i. Suzuki, K. Aizawa, H. Seto, and M.
Arai
SANS Study of Static Structure of The Double Network Polymers
JPS Conference Proceedings 1 14014 (2014)

166 H. Suzuki, S. Harjo, J. Abe, and K. Akita
Influence of Beam Divergence on Pseudo-Strain Induced in Time-ofFlight Neutron Diffraction
Materials Science Forum 777 105-111 (2014)

154 T. Tominaga, S. Takata, J. Suzuki, T. Shinohara, T. Oku, K. Ohishi, T.
Nakatani, Y. Inamura, H. Iwase, T. Ito, H. Kira, K. Suzuya, K. Aizawa,and M. Arai
SANS Study on Double-Network Polymers
JPS Conference Proceedings 1 014014 (2014)

167 K. Ikeda, T. Otomo, H. Ohshita, N. Kaneko, M. Tsubota, K. Suzuya,
F. Fujisaki, T. Ono, T. Yamanaka, K. Shimoda, T. Ichikawa, and Y.
KojimaLocal Structural Analysis on Decomposition Process of LiAl(ND2)4
MATERIALS TRANSACTIONS 55 8 1129-1133 (2014)

155 K. Tsutsumi, M. Fujita, K. Sato, M. Miyazaki, R. Kadono, and K.
YamadaEffects of Oxygen Reduction and Ce-Doping on Magnetic Order in
T'-Pr1.40−xLa0.60CexCuO4+δ−α Studied by μSR Measurement
Key Engineering Materials 616 297-301 (2014)

168 T. Wan, T. Naoe, T. Wakui, M. Futakawa, and K. Maekawa
Cavitation Damage Evaluation Using Laser Impacts
MATERIALS TRANSACTIONS 55 7 1024-1029 (2014)

156 A. J. Clulow, C. Tao, K. H. Lee, M. Velusamy, J. A. McEwan, P. E.
Shaw, N. L. Yamada, M. James, P. L. Burn, I. R. Gentle, and P.
Meredith
Time-Resolved Neutron Reflectometry and Photovoltaic Device
Studies on Sequentially Deposited PCDTBT-Fullerene Layers
Langmuir 30 38 11474-11484 (2014)
157 A. Horinouchi, N. L. Yamada, and K. Tanaka
Aggregation States of Polystyrene at Nonsolvent Interfaces

176

Langmuir 30 22 6565-6570 (2014)

169 W. Gong, K. Aizawa, S. Harjo, J. Abe, T. Iwahashi, and T. Kamiyama
Neutron Diffraction on LPSO Structure in Mg-Zn-Y Alloys
Materials Transactions 54 974-976 (2014)
170 H. Suzuki, K. Kusunoki, Y. Hatanaka, T. Mukai, A. Tasai, M.
Kanematsu, K. Kabayama, and S. Harjo
Measuring strain and stress distributions along rebar embedded inconcrete using time-of-flight neutron diffraction
Measurement Science and Technology 25 2 25602 (2014)
171 Y. Su, Y. Tomota, and S. Harjo

MLF Annual Report 2014

Microstructural Changes by Annealing in Ultrafine-GrainedElectrodeposited Pure Iron
Metallurgical and Materials Transactions A 45 2 990-1000 (2014)
172 Y. Tomota, S. Daikuhara, S. Nagayama, M. Sugawara, N. Ozawa, Y.
Adachi, S. Harjo, and S. Hattori
Stress Corrosion Cracking Behavior at Inconel and Low Alloy Steel
Weld Interfaces
Metallurgical and Materials Transactions A 45 13 6103-6117(2014)
173 Y. Tomota㔞Ꮚ䝡䞊䝮ゎᯒ䜢ά⏝䛧䛯」┦⤌⧊ไᚚ䛸ຊᏛ≉ᛶⓎ⌧䛾ゎ᫂
Microstructural analysis and computational material science formaterials design: applications and future perspectives 87-110(2014)
174 A. Takenaka and Y. Fujii
Elementry Scattering Theory
Morikita Publishing Co. , Ltd. (2014)
175 K. S.-. Ishii, M. Fujita, T. Sasaki, M. Minola, G. Dellea, C. Mazzoli, K.
Kummer, G. Ghiringhelli, L. Braicovich, T. Tohyama, K. Tsutsumi, K.
Sato, R. Kajimoto, K. Ikeuchi, K. Yamada, M. Yoshida, M. Kurooka,
and J. Mizuki
High-energy spin and charge excitations in electron-doped copperoxide superconductors
Nature Communications 5 3714 (2014)
176 I. Klich, S.-H. Lee, and K. Iida
Glassiness and Exotic Entropy Scaling Induced by Quantum
Fluctuations in a Disorder-Free Frustrated Magnet
Nature Communications 5 3498 (2014)
177 A. Machida, H. Saitoh, H. Sugimoto, T. Hattori, A. Sano-Furukawa,
N. Endo, Y. Katayama, R. Iizuka, T. Sato, M. Matsuo, S.-i. Orimo, andK. AokiSite occupancy of interstitial deuterium atoms in face-centred cubiciron
Nature Communications 5 5063_1 - 5063_6 (2014)
178 J. Zhu, S. Du, X. Yu, J. Zhang, H. Xu, S. C. Vogel, T. C. Germann, J. S.
Francisco, F. Izumi, K. Momma, Y. Kawamura, C. Jin, and Y. Zhao
Encapsulation Kinetics and Dynamics of Carbon Monoxide in
Clathrate Hydrate
Nature Communications 5 4128 (2014)
179 M. Hashimoto, E. Nowadnick, R.-H. He, I. Vishik, B. Moritz, Y. He,
K. Tanaka, R. Moore, D. Lu, Y. Yoshida, M. Ishikado, T. Sasagawa, K.
Fujita, S. Ishida, S. Uchida, H. Eisaki, Z. Hussain, T. Devereaux, andZ.-X. Shen
Direct Spectroscopic Evidence for Phase Competition between the
Pseudogap and Superconductivity in Bi2Sr2CaCu2O8+δ
Nature Materials 14 37-42 (2014)
180 M. Hiraishi, S. Iimura, K. M. Kojima, J. Yamaura, H. Hiraka, K. Ikeda,
P. Miao, Y. Ishikawa, S. Torii, M. Miyazaki, I. Yamauchi, A. Koda, K.
Ishii, M. Yoshida, J. Mizuki, R. Kadono, R. Kumai, T. Kamiyama, T.
Otomo, Y. Murakami, S. Matsuishi, and H. Hosono
Bipar tite magnetic parent phases in the iron oxypnictide
superconductor
Nature Physics 10 4 300-303 (2014)
181 M. Igashira, T. Katabuchi, H. Harada, S. Nakamura, A. Kimura, N.
Iwamoto, J. Hori, and Y. Kiyanagi
A Nuclear Data Project on Neutron Capture Cross Sections of LongLived Fission Products and Minor Actinides
Nuclear Data Sheets 118 72-77 (2014)
182 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.

MLF operations in 2014

Igashira, T. Katabuchi, M. Mizumoto, K. Kino, Y. Kiyanagi, T. Fujii, S.
Fukutani, J. Hori, and K. Takamiya
Capture Cross-section Measurement of 241Am(n,γ) at J-PARC/MLF/
ANNRI
Nuclear Data Sheets 119 61-64 (2014)
183 K. Hirose, K. Furutaka, K. Y. Hara, H. Harada, J. Hori, M. Igashira, T.
Kamiyama, T. Katabuchi, A. Kimura, T. Kin, K. Kino, F. Kitatani, Y.
Kiyanagi, M. Koizumi, M. Mizumoto, S. Nakamura, M. Oshima, andY. TohCross Section Measurement of 237Np(n,γ) at J-PARC/MLF/ANNRI
Nuclear Data Sheets 119 48-51 (2014)
184 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
Measurements of Capture Gamma Rays from the Neutron
Resonances of 74Se and 77Se at the J-PARC/MLF/ANNRI
Nuclear Data Sheets 119 128-131 (2014)
185 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, and Y. Toh
A New Signal Processing Technique for Neutron Capture Cross
Section Measurement Based on Pulse Width Analysis
Nuclear Data Sheets 119 398-400 (2014)
186 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
Measurements of Neutron Capture Cross Sections of 112Sn and 118Snwith J-PARC/MLF/ANNRI
Nuclear Data Sheets 119 150-153 (2014)
187 K. 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
Measurement of Capture Gamma Rays from 99 Tc Neutron
Resonances at the J-PARC/ANNRI
Nuclear Data Sheets 119 140-142 (2014)
188 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
Cross Section Measurements of the Radioactive 107Pd and Stable
105,108
Pd Nuclei at J-PARC/MLF/ANNRI
Nuclear Data Sheets 119 143-146 (2014)
189 T. U. Ito, A. Toyoda, W. Higemoto, M. Tajima, Y. Matsuda, and K.
Shimomura
Online full two-dimensional imaging of pulsed muon beams at
J-PARC MUSE using a gated image intensifier
Nuclear Instruments and Methods in Physics Research Section A
754 1-9 (2014)
190 T. Katabuchi, T. Matsuhashi, K. Terada, T. Arai, K. Furutaka, K. Y.
Hara, H. Harada, K. Hirose, J.-i. Hori, M. Igashira, T. Kamiyama, A.
Kimura, K. Kino, F. Kitatani, Y. Kiyanagi, M. Koizumi, M. Mizumoto,
S. Nakamura, M. Oshima, and Y. Toh
Pulse-width analysis for neutron capture cross-section measurement
using an NaI(Tl) detector
Nuclear Instruments and Methods in Physics Research Section A
764 369-377 (2014)
191 N. Kawamura, Y. Irie, H. Fujimori, and Y. Miyake
Development of an ultra low field-ripple electromagnet
Nuclear Instruments and Methods in Physics Research Section A
741 33-36 (2014)177

MLF operations in 2014

MLF Annual Report 2014

192 T. Kawasaki, T. Nakamura, K. Toh, T. Hosoya, K. Oikawa, T. Ohhara,
R. Kiyanagi, M. Ebine, A. Birumachi, K. Sakasai, K. Soyama, and M.
Katagiri
Detector system of the SENJU single-crystal time-of-flight neutron
diffractometer at J-PARC/MLF
Nuclear Instruments and Methods in Physics Research Section A
735 444-451 (2014)
193 K. Kino, M. Furusaka, F. Hiraga, T. Kamiyama, Y. Kiyanagi, K.
Furutaka, S. Goko, K. Y. Hara, H. Harada, M. Harada, K. Hirose, T.
Kai, A. Kimura, T. Kin, F. Kitatani, M. Koizumi, F. Maekawa, S. Meigo,
S. Nakamura, M. Ooi, M. Ohta, M. Oshima, Y. Toh, M. Igashira, T.
Katabuchi, M. Mizumoto, and J. Hori
Energy resolution of pulsed neutron beam provided by the ANNRI
beamline at the J-PARC/MLF
Nuclear Instruments and Methods in Physics Research Section A
736 66-74 (2014)
194 T. Nakamura, M. Katagiri, K. Toh, K. Honda, H. Suzuki, M. Ebine, A.
Birumachi, K. Sakasai, and K. Soyama
A position-sensitive tubular scintillator-based detector as analternative to a 3He-gas-based detector for neutron-scattering
instruments
Nuclear Instruments and Methods in Physics Research Section A
741 42-46 (2014)
195 T. Nakamura, K. Toh, T. Kawasaki, K. Honda, H. Suzuki, M. Ebine, A.
Birumachi, K. Sakasai, K. Soyama, and M. Katagiri
A scintillator-based detector with sub-100-μm spatial resolution
comprising a fibre-optic taper with wavelength-shifting fibre
readout for time-of-flight neutron imaging
Nuclear Instruments and Methods in Physics Research Section A
737 176-183 (2014)
196 M. Nakamura, W. Kambara, Th. Krist, T. Shinohara, K. Ikeuchi, M.
Arai, R. Kajimoto, K. Nakajima, H. Tanaka, J. Suzuki, M. Harada, K.
Oikawa, and F. Maekawa
Feasibility Demonstration of a New Fermi Chopper with
Supermirror-Coated Slit Package
Nuclear Instruments and Methods in Physics Research Section A
737 142-147 (2014)
197 T. Nakamura, A. Ohzu, K. Toh, K. Sakasai, H. Suzuki, K. Honda, A.
Birumachi, M. Ebine, H. Yamagishi, M. Takase, M. Haruyama, M.
Kureta, K. Soyama, H. Nakamura, and M. Seya
Neutron-sensitive ZnS/10B2O3 ceramic scintillator detector as analternative to a 3He-gas-based detector for a plutonium canister
assay system
Nuclear Instruments and Methods in Physics Research Section A
763 340-346 (2014)
198 A. S. Tremsin, T. Shinohara, T. Kai, M. Ooi, T. Kamiyama, Y. Kiyanagi,
Y. Shiota, J. B. McPhate, J. V. Vallerga, O. H. W. Siegmund, and W. B.
FellerNeutron resonance transmission spectroscopy with high spatial andenergy resolution at the J-PARC pulsed neutron source
Nuclear Instruments and Methods in Physics Research Section A
746 47-58 (2014)
199 S. K. Callear, T. Ramirez-Cuesta, K. Kamazawa, S. Towata, T.
Noritake, S. Parker, M. O. Jones, J. Sugiyama, M. Ishikiriyama, andW. I. F. David
Understanding Composition-Property Relationships in Ti-Cr-V-Mo
Alloys for Optimisation of Hydrogen Storage in Pressurised Tanks
Physical Chemistry Chemical Physics 21 16563 (2014)
200 S. Miyatsu, M. Kofu, A. Nagoe, T. Yamada, M. Sadakiyo, T. Yamada,H. Kitagawa, M. Tyagi, V. G. Sakai, and O. Yamamuro
Proton D ynamics of Two -D imensional Oxalate -Bridged
Coordination Polymers
Physical Chemistry Chemical Physics 16 32 17295-17304 (2014)

178

201 K. Amemiya, M. Sakamaki, M. Mizusawa, and M. Takeda
Twisted Magnetic Structure in Ferromagnetic Ultrathin Ni Films
Induced by Magnetic Anisotropy Interaction with Antiferromagnetic
FeMn
Physical Review B 89 054404 (2014)
202 F. Hammerath, P. Bonf`a, S. Sanna, G. Prand, R. De Renzi, Y.
Kobayashi, M. Sato, and P. Carretta
The Poisoning Effect of Mn in LaFe 1−xMn xAsO 0.89F 0.11: Unveilinga Quantum Critical Point in the Phase Diagram of Iron-Based
Superconductors
Physical Review B 89 134503 (2014)
203 M. Hase, M. Soda, T. Masuda, D. Kawana, T. Yokoo, S. Itoh, A.
Matsuo, K. Kindo, and M. Kohno
Experimental confirmation of spin gap in antiferromagnetic
alternating spin-3/2 chain substances RCrGeO5 (R = Y or 154Sm) byinelastic neutron scattering
Physical Review B 90 24416 (2014)
204 K. Kodama, M. Ishikado, S. Wakimoto, K. Kihou, C. H. Lee, A. Iyo, H.
Eisaki, and S. Shamoto
Anisotropic Magnetic Form Factor in a Detwinned Single Crystal of
BaFe2As2
Physical Review B 90 144510 (2014)
205 K. M. Kojima, Y. Krockenberger, I. Yamauchi, M. Miyazaki, M.
Hiraishi, A. Koda, R. Kadono, R. Kumai, H. Yamamoto, A. Ikeda,
and M. Naito
Bulk superconductivity in undoped T'-La1.9Y0.1CuO4 probed by muon
spin rotation
Physical Review B 89 180508(1-5) (2014)
206 J. Lee, S. Demura, M. B. Stone, K. Iida, G. Ehlers, C. R. dela Cruz, M.
Matsuda, K. Deguchi, Y. Takano, Y. Mizuguchi, O. Miura, D. Louca,
and S.-H. Lee
Coexistence of Ferromagnetism and Superconductivity in
CeO0.3F0.7BiS2
Physical Review B 90 224410 (2014)
207 H. Sim, D. C. Peets, S. Lee, T. Kamiyama, K. Ikeda, T. Otomo, S. W.
Cheong, and J.-G. Park
High-resolution structure studies and magnetoelectric coupling ofrelaxor multiferroic Pb(Fe0.5Nb0.5)O3
Physical Review B 90 21 214438 (2014)
208 H. Nakagawa, Y. Yonetani, K. Nakajima, S. Ohira-Kawamura, T.
Kikuchi, Y. Inamura, M. Kataoka, and H. Kono
Local dynamics coupled to hydration water determines DNAsequence-dependent deformability
Physical Review E 90 2 22723 (2014)
209 K. Iida, S.-H. Lee, and S.-W. Cheong
Erratum: Coexisting Order and Disorder Hidden in a Quasi-TwoDimensional Frustrated Magnet
Physical Review Letters 113 079901 (2014)
210 K. M. Kojima, R. Kadono, M. Miyazaki, M. Hiraishi, I. Yamauchi, A.
Koda, Y. Tsuchiya, H. S. Suzuki, and H. Kitazawa
Magnetic Frustration in Iridium Spinel Compound CuIr2S4
Physical Review Letters 112 087203(1-5) (2014)
211 M. Soda, M. Matsumoto, M. Mansson, S. Ohira-Kawamura, K.
Nakajima, R. Shiina, and T. Masuda
Spin nematic interaction in multiferroic compound Ba2CoGe2O7
Physical Review Letters 112 127205 (2014)
212 K. Tomiyasu, K. Iwasa, H. Ueda, S. Niitaka, H. Takagi, S. OhiraKawamura, T. Kikuchi, Y. Inamura, K. Nakajima, and K. Yamada
Spin-Orbit Fluctuations in Frustrated Heavy-Fermion Metal LiV2O4
Physical Review Letters 113 23 236402 (2014)

MLF Annual Report 2014

213 A. M. Dymshits, K. D. Litasov, A. Shatskiy, I. S. Sharygin, E. Ohtani, A.
Suzuki, N. P. Pokhilenko, and K. Funakoshi
P-V-T Equation of State of Na-Majorite to 21 GPa and 1673 K
Physics of the Earth and Planetary Interiors 227 68-75 (2014)
214 E. Ito, D. Yamazaki, T. Yoshino, S. Shan, X. Guo, N. Tsujimo, T.
Kunimoto, Y. Higo, and K. Funakoshi
High Pressure Study of Transition Metal Monoxides MnO and CoO:
Structure and Electrical ResistancePhysics of the Earth and Planetary Interiors 228 170-175 (2014)
215 Y. Shibazaki, H. Terasaki, E. Ohtani, R. Tateyama, K. Nishida, K.
Funakoshi, and Y. Higo
High-Pressure and High-Temperature Phase Diagram for Fe0.9Ni0.1-H
Alloy
Physics of the Earth and Planetary Interiors 228 192-201 (2014)
216 D. Yamazaki, E. Ito, T. Yoshino, N. Tsujino, A. Yoneda, X. Guo, F. Xu, Y.
Higo, and K. FunakoshiOver 1 Mbar Generation in the Kawai-Type Multianvil Apparatus
and Its Application to Compression of (Mg0.92Fe0.08)SiO3 Perovskite
and Stishovite
Physics of the Earth and Planetary Interiors 228 262-267 (2014)
217 W. Chuajiw, K. Takatori, and Y. Fukushima
Polymerization Properties of Polyamide in Bottom-Up Prepared
Polyamide-Calcium Carbonate Composite
Polymer Composites 35 1132–1139 (2014)
218 N. L. YAMADA
Structure Analysis of Polymer Thin Film Using Neutron Reflectometry
POLYMERS 63 2 110-111 (2014)
219 T. Wakui, H. Ishii, T. Naoe, T. Wan, X. Zhihong, K. Haga, H. Takada,and M. Futakawa
Investigation on HIP diffusion bonding of invar alloy and stainlesssteel
Proceedings of International Conference on Hot Isostatic
Pressing'14 210-219 (2014)
220 T. Kai, Y. Kasugai, M. Ooi, H. Kogawa, K. Haga, H. Kinoshita, M.
Seki, and M. Harada
Experiences on radioactivity handling for mercury target system in
MLF/J-PARC
Progress in Nuclear Science and Technology 4 380-383 (2014)
221 M. Kawai, M. Yonemura, S. Torii, T. Muroya, K. Mori, T. Fukunaga, K.
Okuno, K. Takeda, K. Niita, and T. Kamiyama
Novel monolayer shields of a neutron powder diffractometer SPICA
at BL09 of J-PARC
Progress in nuclear science and technology 4 156-159 (2014)
222 K. Okuno, M. Kawai, H. Yamada, T. Shinohara, S. Takata, J. Suzuki, K.
Suzuya, and K. Aizawa
Application of neutron shield concrete to neutron scattering
instrument TAIKAN in J-PARC
Progress in nuclear science and technology 4 619-622 (2014)
223 K. Sakai, T. Kai, M. Ooi, A. Watanabe, T. Nakatani, W. Higemoto, S.
Meigo, S. Sakamoto, H. Takada, and M. Futakawa
Operation status of interlock system of Materials and Life Science
Experimental Facility (MLF) in J-PARC
Progress in nuclear science and technology 4 264-267 (2014)
224 G. A. Beer, Y. Fujiwara, S. Hirota, K. Ishida, M. Iwasaki, S. Kanda, H.
Kawai, N. Kawamura, R. Kitamura, S. Lee, W. Lee, G. M. Marshall,
T. Mibe, Y. Miyake, S. Okada, K. Olchanski, A. Olin, H. Ohnishi, Y.
Oishi, M. Otani, N. Saito, K. Shimomura, P. Strasser, M. Tabata, D.
Tomono, K. Ueno, E. Won, and K. Yokoyama
Enhancement of muonium emission rate from silica aerogel with alaser-ablated surface
Progress of Theoretical and Experimental Physics 091C01(1-7)

MLF operations in 2014(2014)
225 Y. Fukushima and S. Fujita
Dynamics of Confined Water: Proton Dynamics
Radioisotopes 63 381-387 (2014)
226 A. Sano-Furukawa, T. Hattori, H. Arima, A. Yamada, S. Tabata, M.
Kondo, A. Nakamura, H. Kagi, and T. Yagi
Six-axis multi-anvil press for high-pressure, high-temperatureneutron diffraction experiments
Review of Scientific Instruments 85 11 113905 (2014)
227 K. Terada, K. Ninomiya, T. Osawa, S. Tachibana, Y. Miyake, M. K.
Kubo, N. Kawamura, W. Higemoto, A. Tsuchiyama, M. Ebihara,
and M. Uesugi
A new X-ray fluorescence spectroscopy for extraterrestrial materials
using a muon beam
Scientific Reports 4 5072(1-6) (2014)
228 M. Hambsch, H. Jin, A. J. Clulow, A. Nelson, N. L. Yamada, M.
Velusamy, Q. Yang, F. Zhu, P. L. Burn, I. R. Gentle, and P. Meredith
Improved stability of non-ITO stacked electrodes for large area
flexible organic solar cells
Solar Energy Materials and Solar Cells 130 182-190 (2014)
229 D. S. Adipranoto, T. Ishigaki, A. Hoshikawa, K. Iwase, M. Yonemura,
K. Mori, T. Kamiyama, Y. Morii, and M. Hayashi
Neutron diffraction studies on structural effect for Ni-doping in
LiCo1−xNixO2
Solid State Ionics 262 92-97 (2014)
230 T. Hagiwara, K. Nomura, and H. Yamamura
Relationship between crystal structure and oxide-ion conduction
in Nd2Zr2O7 and La2Zr2O7 deduced by high-temperature neutron
diffraction
Solid State Ionics 262 551-554 (2014)
231 Y. Ishikawa, T. Sakuma, H. Takahashi, and S. A. Danilkin
Pressure dependence of crystal structure of Cu2O by TOF powder
neutron diffraction
Solid State Ionics 262 622-624 (2014)
232 E. Kartini, M. Nakamura, M. Arai, Y. Inamura, K. Nakajima, T.
Maksum, W. Honggowiranto, and T. Putra
Structure and dynamics of solid electrolyte (LiI)0.3(LiPO3)0.7
Solid State Ionics 262 833-836 (2014)
233 H. Nozaki, M. Harada, S. Ohta, I. Watanabe, Y. Miyake, Y. Ikedo, N. H.
Jalarvo, E. Mamontov, and J. Sugiyama
Li diffusive behavior of garnet-type oxides studied by muon-spin
relaxation and QENSSolid State Ionics 262 585-588 (2014)
234 N. Tsuchida, S. Harjo, T. Ohnuki, and Y. Tomota
Stress-Strain Curves of Steels
Tetsu-to-Hagane 100 10 1191-1206 (2014)
235 C. A. Tulk, S. Machida, D. D. Klug, H. Lu, M. Guthrie, and J. J.
Molaison
The Structure of CO2 Hydrate between 0.7 and 1.0 GPa
The Journal of Chemical Physics 141 174503 (2014)
236 Y. Kameda, H. Deguchi, H. Furukawa, Y. Kubota, Y. Yagi, Y. Imai, N.
Yamazaki, N. Watari, T. Hirata, and N. Matubayasi
Hydration Structure of CO2-Absorbed 2-Aminoethanol Studied by
Neutron Diffraction with the 14N/15N Isotopic Substitution Method
The Journal of Physical Chemistry B 118 5 1403-1410 (2014)
237 H. Abe, T. Takekiyo, M. Shigemi, Y. Yoshimura, S. Tsuge, T. Hanasaki,
K. Ohishi, S. Takata, and J.-i. Suzuki
Direct Evidence of Confined Water in Room-Temperature Ionic
Liquids by Complementary Use of Small-Angle X-ray and Neutron

179

MLF operations in 2014

MLF Annual Report 2014

Scattering
The Journal of Physical Chemistry Letters 5 7 1175-1180 (2014)
238 T. Naoe and M. Futakawa
Pressure wave-induced cavitation erosion in narrow channel ofstagnant mercury
Transactions of the JSME 80 810 FE0025 (2014)
239 K. Akutsu and T. Ohhara
Application and Outlook of the Pulsed Neutron Beam at J-PARC(1)Introduction of Neutron Beam and Neutron Crystallography at
J-PARCBUNSEKI 2014 11 617-621 (2014)180

MLF Annual Report 2014

Editorial Board

Editorial Board - MLF Annual Report 2014

Chief Editor

Toshiki Asai

Kaoru Sakasai
Neutron Instrumentation Section

CROSS-Tokai

Shin-ichiro Meigo

Takashi Naoe

Facility and Application Development Section

Neutron Source Section

Kaoru Shibata

Asami Sano-Furukawa

Neutron Science Section

Neutron Science Section

Kenji Mishima

Kenji M. Kojima

Neutron Science Section

Muon Science Section

Naritoshi Kawamura

Kenichi Funakoshi

Muon Science Section

CROSS-Tokai

Hiroshi Kira

Kazuhiko Ikeuchi

CROSS-TokaiCROSS-Tokai

181

J-PARC

Japan proton accelerator research complex

High Energy Accelerator Research Organization (KEK)
Japan Atomic Energy Agency (JAEA)

IbarakiTokai

J-PARCJR Joban L ine

Mito
Mt.Tsukuba

Narita

Ueno
Tokyo

0

20

40km

2-4 Shirakata , Tokai-mura, Naka-gun, Ibaraki 319-1195, Japan

http://j-parc.jp/

Materials and Life Science Division
J-PARC Center

http://j-parc.jp/MatLife/en/Comprehensive Research Organization for Science and Society

http://www.cross-tokai.jp/

J-PARC 16-01
KEK Progress Report 2015-5