J-PARC
ANNUALREPORT2 O 1 8Vol.2: Materials and Life Science
Experimental Facility

MLF
ANNUALREPORTMaterials and Life Science Division
J-PARC Center
https://mlfinfo.jp/en
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
https://neutron.cross.or.jp/en

J-PARC 19-02

MLF Annual Report 2018

Preface

PrefaceToshiji Kanaya
Division Head of Materials and Life Science Division, MLF
In fiscal year 2018, the operation of Materials and Life Science Experimental Facility (MLF) started with the neutron
production mercury target (#8), which had helium bubbling system. On April 19, the proton beam power delivered tothe target was increased from 400 kW to 500 kW and the operation continued very stably until July 2, 2018, followed
by a 1-MW test operation for one hour on July 3. The beam availability of the target (#8) to the scheduled beam timewas 92%. In the summer maintenance period, the target was replaced from #8 to #9. The neutron production started
on October 22 and continued stably until March 26, 2019.
The muon rotating target system has been delivering a stable muon beam to users without troubles since 2014.
However, the potential damage of a flexible joint for transferring motor rotation to the graphite disk target has been acause for concern. Some measures were taken to minimize the potential hazards expected in case of suspended target
rotation. By ensuring that those measures were effective, the muon user program was resumed in the beginning ofNovember after two weeks delay behind the original schedule. The operation continued until March 26, 2019, without
troubles.
Due to the stable operation of the facility, the MLF was able to produce many excellent outcomes in various
research fields, such as hard matter, soft matter, energy materials, engineering materials, biomaterials and so on. In
addition to the research outcomes, there were many activities in the MLF in 2018 to enhance the collaboration withinternational and domestic users in academia and various industries. The Annual Meeting of Industrial Application at
J-PARC MLF was held on July 23 and 24 at Akihabara Convention Hall. The total number of attendees has increased to303. The 3rd Neutron and Muon School was held from November 20 to 24. 35 young researchers and graduate students from China, India, Korea, Thailand, Russia, United Kingdom, as well as Japan participated in the school to enjoy
the lectures and hands-on experiments. The 3rd ESS-J-PARC Workshop was held from November 13 to 15. 24 participants from ESS visited J-PARC to exchange information on a wide range of items. On the first day of the workshop, theSwedish Ambassador Magnus Robach delivered his greetings. The Quantum Beam Science Festa, which is a conference mainly for domestic users for MLF J-PARC and IMSS KEK, was held in Tsukuba (EPOCHAL TSUKUBA) on March 12
and 13 with about 580 participants. In this Festa, an MLF symposium was held on March 13 where the MLF facility
status, scientific results and developments were reported.
In the annual report, the research highlights, technical developments and collaboration activities with users in2018 are described in detail.

Materials and Life Science Division, Japan Proton Accelerator Research Complex
https://mlfinfo.jp/enPreface

MLF Annual Report 2018

Preface

Hideaki Yokomizo
Director, CROSSCROSS (Comprehensive Research Organization for Science and Society) has served as a registered institution of
specific neutron beam Facilities of J-PARC appointed by the Government since 2011. We have been supporting theappropriate user program operation of the Public Beamlines at Materials and Life Science Experimental Facility (MLF).
We have also been 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 for bothacademic and industrial researchers. As of 2018, CROSS has four science coordinators who counsel various kinds of users on the neutron sciences and encourage new users in utilizing the neutron beams as advanced and incomparable
research tools.
CROSS supported the user programs at seven fully operational Public Beamlines: BL01 4SEASONS, BL02 DNA, BL11
PLANET, BL15 TAIKAN, BL17 SHARAKU, BL18 SENJU and BL22 RADEN. In 2018, the beam power was operated at 500 kW
using the improved target vessel, which is equipped with pitting protection system. We accomplished a stable andhighly reliable machine operation, which ensured 93% usage of the planned users’ time.
The special program for New User Promotion (NUP) started in 2016 to provide sufficient guidance and assistancefor scientists who are new to the neutron research. NUP has a preferential beam time allocation to first-time or novice
users who need to learn how to use the neutron facility. NUP is expected to cultivate a new scientific field by conducting those users’ first experiments successfully with the sufficient and generous support by our staffs. In the 2017B
proposal round, a new program called Long-Term Proposal was started to select and approve the experimental plansthat will be carried out in a period of three years. Complementary Use is a program that encourages and facilitates
the complementary and collaborative use of pulsed neutrons (J-PARC MLF), synchrotron radiation (SPring-8), and thesupercomputer (K computer).
I hope this Annual Report would serve as a useful information source for anyone wishing to know more about thecurrent status of 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 CROSS, I extend a warm welcome to all researchers who wish to use the Public Beamlines at
J-PARC MLF.

Neutron Science and Technology Center, Comprehensive Research Organization for Science and Society
https://neutron.cross.or.jp/en

Contents
PrefaceOrganization Chart
J-PARC Map
Muon and Neutron Instruments

Research and Development Highlights
Four-Dimensional Mapping of Dirac Magnons ·······································································································································

2

Diffusion Behavior of Methanol Molecules Confined in Cross-Linked Phenolic Resins Studied Using Neutron
Scattering and Molecular Dynamics Simulations ····························································································································

4

Angular Distribution of γ Rays from Neutron-Induced Compound States of 140La ····································································

7

Synthesis, Structure and Magnetic Properties of La0.5Ba0.5CoO2.75+x ································································································· 10
Crystal Structure, Ionic Conductivity and Li-Ion Diffusion Pathway in a La-Li-Co-O System ·················································· 13
High-Speed Neutron Imaging Using a Current-Biased Delay-Line Detector of Kinetic Inductance···································· 15
Symmetrization of Hydrogen Bond in δ-AlOOH under Earth’s Mantle Condition ····································································· 18
Neutron Spin Resonance in the 112-Type Iron-Based Superconductor························································································· 20
Observation of Pressure-Tuned Molecular Reorientational Dynamics in Barocaloric Neopentylglycol ···························· 22
A New Method for Structural Analysis of a Specific Protein or Lipid Membrane in a Molecular-Crowding
Environment Mimicking Living Cells ···················································································································································· 25
Directed Diffusion of Photovoltaic Active Layer Components into Porous ZnO-based Cathode Buffer
Layers in Polymer Solar Cells ··································································································································································· 27
Probing a Unique Spin Texture of 4f Electron Magnet EuPtSi············································································································ 30
In Situ Neutron Diffraction on Phase Transformations for a 1.5Mn-1.5Si-0.2C Steel ································································· 33
Average and Local Structure Analysis of Mn-based Li-ion Cathode Materials by Neutron and Synchrotron X-ray
Sources ············································································································································································································ 37
Deformation Analysis of Reinforced Concrete Using Neutron Imaging Technique··································································· 41
Muon May Reveal the True Worth of “Fool’s Gold” ································································································································· 44
Renormalization of the Spin Excitations in Hexagonal HoMnO3 by Magnon-Phonon Coupling ········································· 46
Structure and Dynamics of Glycine Solution in Mesoporus Silica···································································································· 48
Topological Transitions among Skyrmion- and Hedgehog-Lattice States in Cubic Chiral Magnets···································· 51
2D Bragg-edge Elastic Strain Tomography ··············································································································································· 54
Crystalline Electric Field Level Scheme of the Non-Centrosymmetric CePtSi3 ············································································ 57
Observation of Temperature-Induced Structural Transition of Ceria via Solid-Gas Reaction ················································ 59
Nuclear Magnetic Field Detected with μ±SR ············································································································································ 62

Neutron Source
Progress of the Neutron Source Section ···················································································································································· 66
Operation Status and Design Improvement for the Mercury Target Vessel ················································································· 67
Quadrupole Magnet (QC12) Trouble in 3NBT ·········································································································································· 69

Neutron Science
Neutron Science Section ················································································································································································· 72
BL01: 4D-Space Access Neutron Spectrometer 4SEASONS ················································································································ 74
Current Status of BL02 DNA in 2018···························································································································································· 76
IBARAKI Biological Crystal Diffractometer iBIX········································································································································ 78
Neutron Total Cross Section Measurement at ANNRI (BL04)·············································································································· 80
Status of Fundamental Physics Beamline BL05 (NOP) in 2018 ·········································································································· 82
BL06: Commissioning Status of VIllage of Neutron ResOnance Spin Echo Spectrometers (VIN ROSE)······························ 84
Current Status of BL08 SuperHRPD in 2018·············································································································································· 86
Current Status of SPICA in 2018 ···································································································································································· 88
BL10: NOBORU ···································································································································································································· 90
BL11: Development of Neutron Imaging Technique under High-Pressure Condition ····························································· 91
High Resolution Chopper Spectrometer HRC ········································································································································· 93
BL14 AMATERAS ································································································································································································· 95
Upgrading TAIKAN ····························································································································································································· 96
Installation of Focusing Mirror for Neutron Reflectometry at BL16 SOFIA ··················································································· 97
BL17: Current Status of Polarized Neutron Reflectometer, SHARAKU ···························································································· 100
Status of SENJU 2018 ························································································································································································ 102
TAKUMI and the Engineering Sciences ······················································································································································ 104
The Current Status of the Versatile Neutron Diffractometer, iMATERIA ························································································· 106
Online Analysis System for NOVA································································································································································· 108
Status of the Energy-Resolved Neutron Imaging System RADEN ···································································································· 111
On-Beam Commissioning on POLANO ······················································································································································ 114
3

He Neutron Spin Filter Cells ·········································································································································································· 116

Magnetic Devices and Environment for Polarization Experiment on POLANO ·········································································· 118
Sample Environment at MLF ·········································································································································································· 120
MLF Advanced Computational Environment ·········································································································································· 122
A 200-Micron Spatial Resolution Scintillation Detector for Time-of-Flight Neutron Diffraction Imaging ························· 124Muon Science
Status of J-PARC MUSE: Overview ································································································································································ 128
Report on the Trouble of the Rotation System and the Taken Measures······················································································· 129
Negative Muon at D Line – Beamline Commissioning ························································································································· 132
Development of the Ultra-Slow Muon Beam at the U-line ················································································································· 135
Development of Sample Environment at the S1 Area ·························································································································· 139
H-Line Construction – Recent Progress······················································································································································ 141

MLF Safety
Research Safety ··································································································································································································· 144

MLF Operations in 2018
Beam Operation Status at MLF······································································································································································ 148
Users at the MLF ································································································································································································· 150
MLF Proposals Summary – FY2018 ······························································································································································ 151
MLF Division Staff 2018···················································································································································································· 153
CROSS Staff 2018 ································································································································································································ 156
Proposals Review System, Committees and Meetings ························································································································· 158
Workshops, Conferences, Seminars and Schools in 2018 ··················································································································· 162
Award List ············································································································································································································· 165
MLF Publication 2018 ······················································································································································································· 166

Editorial Board - MLF Annual Report 2018················································································································································ 175

Organization Chart

MLF Annual Report 2018

Organization Chart

Organizaon Chart of
J-PARC Center
Director, J-PARC Center

Organizaon Chart of
CROSS
CROSS is “Registered Instuon for facility Use
Promoon” for the public-access neutron
beam facilies at J-PARC.

Deputy Director (JAEA, KEK, Safety)
President

Safety Division
CROSS Head Oﬃce

Accelerator Division
Research Center for
Science and Society

Materials & Life Science Division

Neutron Science andTechnology Center

Neutron Source SeconDirector, Neutron Scienceand Technology Center

Neutron Science Secon

Science Coordinators

Neutron InstrumentaonSeconR&D Division

Muon Science SeconTechnology Development
SeconUlizaon Promoon
Division
Safety Division
Administraon DivisionParcle & Nuclear Physics Division
Nuclear Transmutaon Division
Cryogenics SeconInformaon System SeconAdministraon Division
Users Oﬃce

The Role of CROSS
Under the terms of the legislation that supports the
Public Neutron Beam Facility, CROSS is entrusted withspecific responsibilities. In practical terms, the corefunctions of CROSS can be summarized as follows:• 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 2018

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

J-PARC Center Users Oﬃce

R245

KEK Tokai Campus

Main Gate
R245

Linac

HENDEL R&D Building

3 GeV Synchrotron

MLF

50 GeV Synchrotron

J-PARC Research Building

J-PARC Map

25 m

1m

As of March 2019

MLF Annual Report 2018

400 ｍmMuon and Neutron Instruments

Research and Development
Highlights

Research and Development Highlights

MLF Annual Report 2018

Four-Dimensional Mapping of Dirac Magnons
1. Introduction
Following the remarkable discovery of topologicalinsulators, exploration of topological band structures incrystalline materials has been a topical line of research incondensed matter physics. The notion of band topology
lies in the mapping from momentum space, which follows from the lattice translational symmetry, to Hilbert
space, which follows from the fact that band structures
can be understood as solution to an eigen-value problem. Importantly, topological bands are not restricted
to fermions as the constituent (quasi)particles. Since theexistence and categorization of topological bands depend on symmetry and dimensionality, prediction andexperimental discovery of topological bands of classicaland bosonic excitations have been an active line of research in recent years – they offer more possibilities ofsymmetry that can be materialized realistically.
In 2017, we predicted [1] that there can be a (backthen) new type of Dirac points in the band structure ofmagnons in three-dimensional antiferromagnets with
PT and U(1) symmetry. The U(1) symmetry requires
collinear magnetic structure, and the PT symmetry requires that the material has inversion symmetry which
relates up-spin sub-lattice to down-spin sub-lattice.
Importantly, the prediction can in principle apply to alarge class of materials, and a specific example was recognized: Cu3TeO6. This is a material that can be grown(a)into large single crystals and hence suitable for inelastic
neutron scattering experiments for verifying the theoretical predictions. At J-PARC, we have successfully performed such experiments and confirmed the theory [2].
The experimental data were very clean and they provedthat there are long-range spin interactions in the system, which suppress quantum fluctuations and facilitate the observation of highly harmonic magnon bands.
2. Technical Advantages
There are several advantages of using time-offlight inelastic neutron scattering (ToF-INS) to determine band topology: (1) ToF-INS can reliably measureband structures with good momentum resolution in
all three dimensions, in contrast to ARPES which has
limited resolution perpendicular to the sample surface;(2) the scattering matrix elements are quantitatively
known, therefore S(Q,w) can be used to verify the theoretically predicted wave functions which are the carrierof the non-trivial topology; (3) for materials with highcrystallographic symmetry, cubic symmetry in particular, the 4-dimensional data set obtained by ToF-INS canbe folded according to the symmetry, in which way thestatistical accuracy can be greatly improved.
Our experiment was carried out on the highflux thermal ToF-INS spectrometer BL-01 (4SEASONS)at the MLF. Figure 1 displays an overview of our(b)Figure 1. (a) Illustration of symmetry-allowed folding of Tof-INS data into the physically meaningful sector (indicated by red dottedlines), which contains many different Brillouin zone sectors. Intensity as functions of energy and momentum transfer along
the high-symmetry lines (colored dotted lines) of the Brillouin zone sectors are displayed as contour plots in the insets thatsurround the main figure. (b) Comparison between theoretical calculation (middle panel) and experimental data (bottom
panel) for a given Brillouin zone along high-symmetry lines, showing excellent agreement.

2

MLF Annual Report 2018

symmetry-folded data set that contained S(Q,w) information for many different Brillouin zone sectors. As thedispersion relationship has to be identical in all these
sectors but the intensity can vary, these data can beused to over-determine the theoretical model’s interaction parameters. The outcome of the global fitting is
extremely satisfactory, and we are able to reproduce
the experimentally observed S(Q,w) to a high level ofaccuracy (Fig. 1(b)).
3. Visualization of a Topological Dirac Point
After the theoretical model was successfully fittedusing the highly accurate 4D experimental data set, weused the model to precisely predict favorable locations
for observing the topological magnon Dirac points.
One of such points was predicted to be P(1.5, 0.5, 1.5)
near 17.8 meV (Fig. 2), and indeed, by sufficiently utilizing the statistical accuracy of the data allowed (again)
by symmetry-related folding, we were able to obtaina sub-resolution visualization of the magnon Diracpoint in constant-E slices that were separated by only
0.2 meV (compared to FWHM energy resolution of
about 0.58 meV). The dispersion near the Dirac point isevident from these data.
4. Future Plans
For the Cu3TeO6 system, we estimate that what
we have successfully observed is essentially what canbe resolved by today’s state-of-the-art instrumentation. Generally speaking, the INS technique can be further used to visualize topological bosonic excitations’wave-function structure, e.g., by using spin-polarized
neutrons to measure magnons. In addition, it remains

Research and Development Highlights

(b)

(a)

Figure 2. (a) Theoretical calculation of magnon dispersion
near a Dirac point at the Brillouin zone P-point at
about 17.8 meV. (b) Experimental intensity profiles
generated by symmetrizing ToF-INS data at P(1.5,
0.5, 1.5) and plotting them in constant-E slices.

a technical challenge to measure the topological magnon surface states, as well as to observe topologicalmagnons’ transport properties such as topologicalthermal Hall effects. We have on-going collaborations
for these purposes involving the use of our high-quality
Cu3TeO6 single crystals.
References[1] K. Li et al., Phys. Rev. Lett. 119, 247202 (2017).
[2] W. Yao et al., Nat. Phys. 14, 1011 (2018).

Yuan Li1, Weiliang Yao1, Kazuki Iida2, and Kazuya Kamazawa2International Center for Quantum Materials, Peking University, China; 2Neutron Science and Technology Center, CROSS

1

3

Research and Development Highlights

MLF Annual Report 2018

Diffusion Behavior of Methanol Molecules Confined in
Cross-Linked Phenolic Resins Studied Using Neutron
Scattering and Molecular Dynamics Simulations

2. Experimental
We prepared highly deuterated cross-linked phenolic resins via two processes: synthesis of deuterated
novolac resin from phenol-d6 and formaldehyde-d2
under acidic condition, and subsequent crosslink reaction using hexamethylenetetramine (HMTA) as a curing
agent [3]. After molding, cured phenolic resin (dNVH)
and solvent (CH3OH or CD3OD) were sealed in a pressure vessel and allowed to stand for 72 hours in an 80°C
oven. Then, the sample was dried in the air and pulverized with a mill for QENS measurement. The amount ofpenetrant methanol in the sample was estimated to beabout 8 wt% from the weight change measurement
value after heating in a vacuum oven. From the composition of dNVH and methanol in dNVH–CH3OH, theratio of incoherent scattering cross-sections (σinc) is estimated to be σinc (HdNVH) : σinc (DdNVH) : σinc (HCH3OH)  6.9 : 1 :4

11.1. This suggests that sufficient incoherent scattering
intensity from the CH3OH in the dNVH–CH3OH can beobtained by the QENS measurement for dNVH–CH3OH.
QENS experiments were performed using thetime-of-flight near-backscattering spectrometer installed at J-PARC/MLF BL02 DNA [4]. Powder samples
were lapped with thin aluminum foil and loaded in acylindrical aluminum sample holder. The dynamic scattering functions S(Q, ω) were measured at 296 K, in a
momentum transfer range 0.1  Q  1.8 Å1. The energy
window and resolution were 40 eV  ħω  100 eVand E  3.6 eV, respectively. The QENS data reduction
and analyses were performed using software provided
by the DNA group of J-PARC/MLF.
3. Results and Discussion
Figure 1 shows the measured QENS profiles ofdNVH–CH3OH, dNVH–CD3OD, and dried dNVH normalized by the elastic intensity at Q  1.7 Å1. The difference in scattering intensity between dNVH–CH3OH anddNVH–CD3OD indicates the existence of quasi-elastic
broadening from methanol. Furthermore, the intensity in dNVH–CD3OD, larger than that of dried dNVH in
the quasielastic region, implies the induction of resin
dynamics derived from solvent invasion. Accordingly,
the QENS profile of dNVH–CH3OH is represented by thesum of methanol and dNVH components as follows:101
Q = 1.7 Å−1 , T = 296 K
dNVH–CH3OH
dNVH–CD3OD
dNVH (dry)resolution

100

S(Q,ω) / a.u.

1. Introduction
Phenolic resin is a thermosetting polymer widelyused in many industrial applications, such as automobiles, semiconductors, and aerospace equipment. Its
excellent properties, such as strong mechanical properties, thermal stability, electric resistance, and solvent
resistance, are due to the dense chemically bonded
network structure [1]. These applications, especially automotive parts and semiconductor packages, require
high solvent resistance because they may be exposed
to various solvents under prolonged conditions of hightemperature and pressure. Solvent penetration into thecured thermosetting resins causes many problems, including dimensional changes, decreases in mechanicalstrength and modulus leading to solvent stress cracking, and short-circuiting. In designing thermosetting
materials, it is necessary to understand the relationships
between a cross-linked structure and solvent resistancefrom the perspective of atomistic structure. Elucidationof the diffusion mechanism of small molecules, such as
water, methanol, or ethanol, in cured resins is of special
importance for achieving high solvent resistance [2]. In
this study, we investigated the diffusion dynamics ofmethanol confined in highly cross-linked phenolic resins using quasi-elastic neutron scattering (QENS) andatomistic molecular dynamics (MD) simulations.

10−1

10−2

10−3
−20

0

20

40

60

80

ħω / μeV

Figure 1. Typical QENS spectra for dNVH–CH3OH, dNVH–
CD3OD, and dried dNVH at Q = 1.7 Å−1. The spectra
are normalized by the elastic intensity.

MLF Annual Report 2018

M
S(Q, ω)  [AMel (Q)δ(ω)  Aqe(q)LM(Q, ω)  ARel(Q)δ(ω) RR
Aqe(q)L (Q, ω)] R(Q, ω)  bkg.,
where R(Q, ω), δ(ω), and L(Q, ω) are the resolution function of the DNA spectrometer, the delta function, andthe Lorentz function, respectively, and bkg. denotes the
background. Ael, and Aqe denote the coefficients of eachscattering component for elastic and quasielastic scatterings, and superscripts M and R indicate methanoland cured resin (dNVH), respectively.
Figure 2 shows the Q2-dependence of , whereindicates the HWHM in the Lorentz function of methanol. The Q-dependency of for methanol in cured resin
closely followed a fitting curve of the random-jumpdiffusion model,  DQ2 / (1  τ0DQ2), though the continuous diffusion model,  DQ2, did not match in thehigh-Q range. Here D is the translational diffusion coefficient. The fitting results in D  1.6 106 cm2/s formethanol confined in cured resin, which is one order ofmagnitude smaller than the value in the bulk, D  2.3
105 cm2/s.
Full atomistic MD simulations were carried out on
the methanol dispersed cross-linked phenolic resin
model systems. The details of the MD simulation were
described in references [4–6]. Figure 3 shows a 3D image of methanol dispersed in a cross-linked phenolic
resin. Methanol molecules in the resin network reside
in void spaces near hydroxyl groups of phenolic units
form hydrogen bonds to the phenolic hydroxyl groupor other methanol molecule.
Figure 4 shows the trajectory lines of 20 randomly chosen methanol molecules in 2 ns acquired every

Research and Development Highlights

10 ps. These molecular trajectories in the MD simulation clearly indicate that some methanol molecules diffuse by moving a small distance in a limited space,although most methanol molecules are not moving.
Such a leaping movement corresponds well to the
jump-diffusion model, as suggested from the QENS
results. Furthermore, the diffusion coefficient D of diffusive methanol was estimated from the time dependence of the mean squared displacement using Einstein’s
relation. The estimated D for diffusive molecules is 1.63

69.6 Å

69.8 Å
68.5 Å
Figure 3. 3D model of methanol molecules (yellow), confined in cured phenolic resins (blue), used in the
MD simulation.

1.86×10−630
0.0031×10−6

simple diffusion

25

1.39×10−6
0.499×10−620

Γ / μeV0.274×10−6150.370×10−6

4.07×10−6

10jump diffusion
0.0152×10−6

5
0

y

0

1

2

3

4

Q2 / Å–2
Figure 2. Q2-dependence of Γ of CH3OH for dNVH–CH3OH
obtained from QENS fitting at T = 296 K. The redand blue lines are fitting results by the simple-diffusion and jump-diffusion models, respectively.

x

1.10×10−6

Figure 4. Representative trajectory lines of methanol molecules in 2 ns acquired every 10 ps. The values
shown close to the particles indicate D (cm2/s).
Lines of non-diffusive methanol are shown in blue,
and lines of diffusive methanol are displayed withdifferent colors.

5Research and Development Highlights

MLF Annual Report 2018106 cm2/s, which is well consistent with the QENS experiments, i.e., D  1.6 106 cm2/s. This agreement suggests that our constructed MD model is very reasonable
and the existence of confined dynamics for methanol ishighly probable.
Acknowledgements
The QENS experiments were executed using theBL02 (DNA) beamline at the Materials and Life Science
Experimental Facility (MLF) of J-PARC under Proposal
No. 2015A0077 and 2016A0177. This research used
computational resources of the K computer provided
by the RIKEN Advanced Institute for Computational
Science through the HPCI System Research project(Project ID: hp160089).

References[1] J.-P. Pascault, H. Sautereau, J. Verdu, R. J. J. Williams,
Thermosetting Polymers; Marcel Dekker: New York,2002.
[2] M. L. Kaplan, Polym. Eng. Sci., 31, 689 (1991).
[3] A. Izumi, T. Nakao, and M. Shibayama, J. Polym. Sci.
A., 49, 4941 (2011).
[4] Y. Shudo, A. Izumi, K. Hagita, T. Yamada, K. Shibata
and M. Shibayama, Macromolecules, 51, 6334
(2018).
[5] Y. Shudo, A. Izumi, K. Hagita, T. Nakao, and M.
Shibayama, Polymer, 103, 261 (2016).
[6] Y. Shudo, A. Izumi, K. Hagita, T. Nakao, and M.
Shibayama, Polymer, 116, 606 (2017).

Y. Shudo1, A. Izumi1, K. Hagita2, T. Yamada3, K. Shibata4, and M. Shibayama5
Corporate Engineering Center, Sumitomo Bakelite, Co., Ltd.; 2Department of Applied Physics, National Defense Academy of Japan; 3Neutron
Science and Technology Center, CROSS; 4Neutron Science Section, Materials and Life Science Division, J-PARC Center; 5Neutron Science
Laboratory, Institute for Solid State Physics, The University of Tokyo

1

6

MLF Annual Report 2018

Research and Development Highlights

Angular Distribution of γ Rays from Neutron-Induced
Compound States of 140La
1. Introduction
Very large parity violations with a maximum size of1 have been observed in several compound nuclei
10
formed after neutron capture by several nuclides suchas 139La, 131Xe, 117Sn, and 81Br [1]. It is theoretically understood that the tiny parity violation with the size of 107caused by the weak interaction is enhanced by up to
106 with the interference between s- and p-wave amplitudes. This hypothesis is referred to as s-p mixing. The
parity violation in the compound nuclei is describedwith the weak matrix element W and a ratio of the partial
neutron width of the p-wave resonance x. Additionally,an enhancement of the time reversal (T) violation in
the compound nucleus can also be calculated using x.
A T-violating cross section T in the compound nucleus is described as [2]
WT
P ,
W
where P is the P-violating cross section in the compound nucleus, W T is the T-violating matrix element,and κ(x) is the spin factor, corresponding to a conversion constant from the P-violating cross section to the
T-violating cross section. Since the T-violation can bea key to reveal the origin of our matter-dominant universe under the assumption of CPT theorem [3, 4], κ(x)is an important parameter to evaluate the potential tosearch for a new physics.
Therefore, x and W are essential parameters for the
study of the discrete symmetry violation in the compound nuclei. The product of W and x has been measured in several nuclei, however, the individual values ofx and W have not yet been determined. The value of x
can be extracted from the neutron energy dependenceof the angular distribution of the -rays from the p-wave
resonance of the compound nucleus [5]. We conducted
an experiment to measure the angular distributions ofthe -rays from the 0.74 eV p-wave resonance of the139
La, where an extremely large parity violation with thesize of the (9.56  0.35)% was observed [6].
T  κ(x)2. Experiment and result
The experiment was performed using a germanium
detector assembly in BL04, ANNRI. The Germanium detector assembly consists of 22 individual germanium
crystals, whose angles are 36°, 71°, 72°, 90°, 108°, 109°,

and 144° with respect to the direction of the incident
neutron momentum. A natLa plate with the dimensionsof 40 40 1 mm was used as a sample. The measurement time was 60 h, and the average beam power was
150 kW during the experiment. We investigated the angular distribution of -rays with the energy of 5161 keV,which is the Q value of the 139La+n state. Figure 1 shows
the neutron spectra in the vicinity of the 0.74 eV pwave resonance gated with the full absorption peakof 5161 keV -rays. We can see that the shape of the pwave resonance is distorted according to the detector
angle. Note that the neutron spectrum was divided by
the incident neutron spectrum measured using a 10B
sample and the background caused by the Compton
scattering from the high energy -rays was subtracted.
The detection efficiencies of each detector were corrected by constructing a GEANT 4 simulation [7].
3. Analysis
In order to quantify the distortion of the peak, wedefined the asymmetry of the p-wave resonance withrespect to the peak energy ALH as
NL  NH,
NL  NH
where NL and NH are the integral values of the neutron
spectrum in the region of low energy (0.66–0.74 eV)and high energy (0.74–0.82 eV), respectively. The angular distribution of the ALH is shown in Fig. 2. We foundthe clear angular dependence in the -rays from the
0.75 eV p-wave resonance to the ground state of 140La
as shown in Fig. 2.
The angular distribution of ALH was analyzed bycomparing it to a theoretical calculation based on thes-p mixing model. Finally, the values of x and W wereobtained as0.04
x = 0.160.09
0.11, 0.950.03,
18.1
0.10)meV.
W  (13.25.3 )meV, (2.210.06
The value of κ(x) was also determined using thevalue of x as
0.08
κ(x) = 4.845.58
1.69, 0.990.07.
The fact that κ(x) is the order of 1 implies that the
T-violation is also enhanced by an order of 106 as theP-violation in the compound state of 140La. This resultshows that 139La would be a strong candidate for the
T-violation search experiment.
ALH 

7

MLF Annual Report 2018

θ γ = 108 deg

3
2
1
0
0.2

0.4

0.6

0.8

1

1.2

θ γ = 90 deg

4
3
2
1
0
0.2

1.4

0.4

0.6

1.2

90°

3

108°
109°

1

0.6

0.8

1

1.2

72°
71°

144°

3
2

Downstream
1

0.6

0.8

1

1.2

0.8

1

1.4

θ γ = 71 deg

4
3
2
1

0.4

0.6

0.8

1

1.2

1.4

E lap [eV]5θ γ = 36 deg

4
3
2
1
0
0.2

1.4

E lap [eV]

1.2

5

36°

θ γ = 144 deg

0.4

0.6

0
0.2

5

0
0.2

0.4

1.4

E lap [eV]41

E lap [eV]

2

0.4

2

E lap [eV]θ γ = 109 deg

4

3

0
0.2

1.4

5

0
0.2

∂ I γ / ∂ E lap [arbitrary unit]1θ γ = 72 deg

4∂ I γ / ∂ E lap [arbitrary unit]∂ I γ / ∂ E lap [arbitrary unit]

E lap [eV]0.85

∂ I γ / ∂ E lap [arbitrary unit]

45∂ I γ / ∂ E lap [arbitrary unit]

5∂ I γ / ∂ E lap [arbitrary unit]∂ I γ / ∂ E lap [arbitrary unit]

Research and Development Highlights

0.4

0.6

0.8

1

1.2

1.4

E lap [eV]

Figure 1. The neutron energy spectra in the vicinity of the 0.74 eV p-wave resonance for each detector angle. The central figure
denotes each crystal of the detectors and its degrees. The valuable of Iγin the vertical axis corresponds to the number ofdetected γ-rays.

0.2

0

−0.2

−0.4
−1

−0.5

0

0.5

1

Figure 2. Angular dependence of ALH. The sold line shows thebest fit with a linear function.

8

4. Future plans
We limited x to the two values by conducting
the measurement using the unpolarized neutrons.
However, a measurement of the angular distribution ofthe -rays using polarized neutrons is necessary to finally determine the value of x. We have already complete
the experiment using a 3He spin filter in ANNRI [8], andthe analysis is currently ongoing. Additionally, measurements of the angular distribution of the -rays withother nuclides such as 117Sn [9], 81Br, 131Xe, 111Cd, 113In,
and 127I, which have enhanced P-violations, also are under way.
Our final goal is to search for an unknown
T-violating effect in the compound nuclei. Several developments such as a polarized La target, the neutron
polarizer, and a neutron detector [10] also are startingfor the T-violation search experiment.

MLF Annual Report 2018

References[1] G.E.Mitchell et al., Phys. Rep. 354, 157 (2001).
[2] V. P. Gudkov, Phys. Rep. 212, 77 (1992).
[3] A. D. Sakharov. JETP Lett., 5, 24, (1967).
[4] J. Schwinger. Phys. Rev., 91. 713, (1953).
[5] V. V. Flambaum et al., Nucl. Phys. A 435, 352–380(1985).

Research and Development Highlights[6] V. P. Alfimenkov et al., Nucl. Phys. A 398, 93 (1983).
[7] S. Takada et al., Journal of Instrumentation 13,
P02018 (2018).
[8] T. Yamamoto et al., JPS Conf. Proc. 22, 011018(2018).
[9] J. Koga et al., JPS Conf. Proc. 22, 011035 (2018).
[10] S. Endo et al., JPS Conf. Proc. 22, 011021 (2018).

T. Okudaira1, S. Takada2, K. Hirota3, A. Kimura4, M. Kitaguchi3, J. Koga2, K. Nagamoto3, T. Nakao4, A. Okada3, K. Sakai5, H. M. Shimizu3,
T. Yamamoto3, and T. Yoshioka2
1
Technology Development Section, Materials and Life Science Division, J-PARC Center; 2Kyushu University; 3Nagoya University; 4Nuclear
Data Center, Nuclear Science and Engineering Center, JAEA; 5Neutron Source Section, Materials and Life Science Division, J-PARC Center9Research and Development Highlights

MLF Annual Report 2018

Synthesis, Structure and Magnetic Properties of
La0.5Ba0.5CoO2.75+x
1. Introduction
The cobaltite perovskites exhibit many unusual
properties such as spin-state transition, metal–insulator transition, large magnetoresistance, negative thermal
expansion and so on [1–4]. The coupling between thelattice, charge, orbital, and spin degrees of freedom isfound to play an essential role. For example, LaCoO3 with
the Co valence being 3, exhibits the spin-state transition upon heating, from the low-spin (LS) state (t2g6,
S  0) to the high-spin (HS) state (t2g4eg2, S  2) via theintermediate-spin (IS) state (t2g5eg1, S  1) [1, 5].
The hole-doping effect to LaCoO3 has been researched extensively through substitution of divalent
ion A (A  Ca, Sr, Ba) for La [6]. It is well established that
the LS nonmagnetic ground state of LaCoO3 undergoes a transition to IS or HS ferromagnetic (FM) state in
La1xAxCoO3 [7]. Also, a large magnetoresistance effect
was reported in La1xAxCoO3 [3].
However, hole doping to Co3 ion can also be introduced by changing the oxygen content, which has notbeen widely exploited. For example, the nominal valenceof Co ion in La0.5A0.5CoO2.75 is 3, and holes can be filled tothe band by increasing the oxygen content. In a previous
report [8–11], the A-site disordered La0.5Ba0.5CoO2.75x (x 0.25), shows FM transition at Curie temperature (TC)190 K. As the doping decreases to x  0.12, the antiferromagnetic (AFM) correlation develops while the FM statesurvives at base temperature. When the oxygen content
is further lowered to an electron doping side (x  0.15),
it shows pure AFM state with the Neel temperature (TN)above room temperature.
Since the properties of cobaltite perovskites arevery sensitive to external stimulus (temperature, pressure, etc.) or chemical compositions (rare-earth element, oxygen content etc.), we synthesized the sample
La0.5Ba0.5CoO2.75x with lighter hole doping level (x  0.08
and x  0.16) and characterized their magnetic properties. We found that sample x  0.08 shows a magnetic
behavior similar to the one of sample x  0.05, but whencompared with sample x  0.12, a slight increase of thedoping to x  0.16 leads to the change from two phaseswith long range AFM and FM ordering to only one phasewith long range FM ordering.
2. Experiment method
The samples of La0.5Ba0.5CoO2.75x were synthesized
10

by standard solid-state reaction. The raw materials La2O3,
BaCO3 and CoO were ground, pressed into a pellet andheated at 1200°C in air for 12 h. After grinding and heating were repeated 3 times, we could obtain the pureA-site disordered La0.5Ba0.5CoO2.75x (x  0.16). The samplex  0.08 was obtained by annealing the attained sample
under Ar flowing at 250°C for 12h. The oxygen content
was determined by analysis of the neutron powder diffraction (NPD) pattern.
The high-resolution NPD measurement was
performed by the Super High Resolution Powder
Diffractometer (SuperHRPD) at MLF, J-PARC. The neutron diffraction patterns were analyzed by the Rietveld
refinement method using both Z-Rietveld [12] andFULLPROF [13], and the representation analysis was
utilized by SARAh [14]. The magnetization under fieldcooled (FC) and zero-field cooled (ZFC) was investigatedby using superconducting quantum interference device(SQUID) magnetometer (MPMS) at the Cross-Tokai user
laboratories.
3. Results and discussion
Figure 1 shows the temperature dependence ofmagnetization for x  0.08 and x  0.16 under 100 Oe.
The FC magnetization [see Fig. 1(b)] of x  0.16 exhibitsa ferromagnetic transition at about 160 K. For sample x
 0.08, below 130 K the decrease of FC magnetization
upon cooling indicates the AFM state at low temperature. However, the divergence between the magnetization of ZFC and FC in Fig. 1(a) and the hysteresis loop of
the M/H curve [see the inset] at 13 K suggest that FM correlation also exists at low temperature. From the viewpoint of the phase diagram, x  0.08 is located near thephase boundary of AFM and FM, therefore it is natural tosee the coexistence of AFM and FM state, which comesfrom the electronic origin. Since it is in the vicinity ofthe boundary, the energy of the AFM and FM states isvery close.
As shown in Fig. 2, the superlattice reflections (1/2
1/2 1/2) initiated at TN  210 K signify the AF orderingwith propagation vector kAFM  (1/2, 1/2, 1/2), while theincrease in intensity of the reflection (100) initiated fromTC  160 K upon cooling, indicates the ferromagnetic ordering with propagation vector kFM  (0, 0, 0).
The pattern of sample x  0.08 can be fitted well by
the Pm3̅m cubic structure with the G-type AFM structure,MLF Annual Report 2018(a) 100

40

T = 10 K

0.00
-0.03
-0.06
-10000 -5000

ZFC

05000 10000
H (Oe)M (emu/mol)

60

1200

ZFC

800

1

T = 10 K

0-1-10000 -5000

05000 10000
H (Oe)400

200

H = 100 Oe
x = 0.16

FC

0.06
0.03

1600

M (μB/Co)FC
M (μB/Co)M (emu/mol)

80

(b)

H = 100 Oe
x = 0.08

Research and Development Highlights

0
50

100

150

200

250

50

300

100

T (K)

150

200

250

300

T (K)

Figure 1. Temperature dependence of magnetization for La0.5Ba0.5CoO2.75+x (a) x = 0.08 and (b) x = 0.16.under 100 Oe in the ZFC and
FC processes. The inset shows the M/H curve at 10 K.

(b)

x = 0.08(1/2 1/2 1/2 )4030

Integrate intensity (arb. unit)

Integrated intensity (arb. unit)(a) 50

TN

20
10
0

25

x = 0.16(1 0 0)

20

TC

15
10
5
0

0

50

100

150

200

250

300

T (K)

0

50

100

150

200

250

300

T (K)

Figure 2. The temperature dependence of integrated intensity of (a) AFM reflection (1/2 1/2 1/2) for La0.5Ba0.5CoO2.75+x (x = 0.08) and(b) the FM reflection (1 0 0) for La0.5Ba0.5CoO2.75+x (x = 0.16). The inset of (a) and (b) shows the G-types AFM and FM structure,
respectively. For clarity, only Co is displayed.

as shown in Fig. 3(a). In the G-type AFM structure, every
Co ion aligns antiparallelly with the nearest Co neighbors, as shown in the inset of Fig. 2(a). As mentioned
above, the magnetization of the x  0.08 sample suggests the existence of FM correlation. Throughout thetemperature range, we did not observe any ferromagnetic reflection in the NPD pattern, indicating that there
is no long-range FM ordering. Therefore, we think that
the FM correlation occurs in forms of short-range ordering together with a long-range AFM ordering at low temperature for sample x  0.08.
Similarly, the simple FM structure found for x  0.16 is
depicted in the inset of Fig. 2(b) and the fitted pattern isshown in Fig. 3(b). In the NPD pattern of La0.5Ba0.5CoO2.75x(x  0.16) at low temperature we could not observe

reflections (1/2 1/2 1/2) and (3/2 1/2 1/2). So, there is
no long-range ordered AFM state at low temperature inthis sample. It has been reported that FM state and small
AFM clusters coexist in ground state in La0.5Ba0.5CoO2.75x(x  0.25) [15]. In the case of x  0.16, a short-range ordered AFM state, which cannot be detected by NPD,
may coexist with the long-range ordered FM state at low
temperature as well. In order to clarify whether thereis short-range ordered AFM state at low temperature,
further experiments are needed, such as the muon-spinrelaxation experiment.
4. Conclusion
We synthesized the A-site disordered La0.5Ba0.5CoO2.75x(x  0.08 and 0.16) and investigated the crystal and11Research and Development Highlights

MLF Annual Report 2018

(a)

(b)

Figure 3. The NPD patterns of La0.5Ba0.5CoO2.75+x (a) x = 0.08, (b) x = 0.16 were collected at 13 K. The observed and calculated patterns
are shown at the top with the cross markers and the solid line, respectively. The vertical green and purple marks in the
middle show the calculated positions of Bragg reflections for nuclear and magnet diffraction, respectively. The bottom
blue line represents the difference between observed and calculated intensities. The inset illustrates the cubic perovskite
with the space group Pm3̅ m.

magnetic structures of the samples by magnetizationand high-resolution NPD. By analyzing the NPD data,
we found that the crystal structures remain in the cubic structure with space group Pm3̅ m in the wholetemperature range. Sample x  0.16 shows FM state at
low temperature with the transition at 160 K. For the x 0.08 sample, the short range ordered FM state occurs
together with a long-range ordered AFM state at low
temperature.
References[1] M. A. Señarís-Rodriguez and J. B. Goodenough, J.
Solid State Chem., 116, (1995) 224.
[2] Y. Moritomo, M. Takeo, X. J. Liu, T. Akimoto and A.
Nakamura, Phys. Rev. B, 58, (1998) R13334.
[3] G. Briceño, H. Chang, X, Sun, P. G. Schultz, and X. D.
Xiang, Science, 270, (1995) 273.
[4] P. Miao, X. Lin, A. Koda, S. Lee, Y. Ishikawa, S. Torii,
M. Yonemura, T. Mochiku, H. Sagayama, S. Itoh,
K. Ikeda, T. Otomo, Y. Wang, R. Kadono, and T.
Kamiyama, Adv. Mater., 29, (2017) 1605991.
[5] T. Saitoh, T. Mizokawa, A. Fujimori, M. Abbate, Y.
Takeda, and M. Takano, Phys. Rev. B, 55, (1997)
4257.
[6] M. Kriener, M. Braden, H. Kierspe, D. Senff, O.

Zabara, C. Zobel, and T. Lorenz, Phys. Rev. B, 79,(2009) 224104.
[7] M. A. Señarís-Rodriguez and J. B. Goodenough, J.
Solid State Chem., 118, (1995) 323.
[8] T. Nakajima, M. Ichihara and Y. Ueda, J. Phys. Soc.
Jpn., 74, (2005) 1572–1577.
[9] V. Sikolenko, V. Efimov, I.O. Troyanchuk, D.V.
Karpinsky, M.V. Bushinsky and D. Sheptyakov, J.
Phys. Conf. Ser., 391, (2012) 012106.
[10] I.O. Troyanchuk, M.V. Bushinsky, V. Sikolenko, V.
Efimov, C. Ritter, T. Hansen, and D.M. Többens, Eur.
Phys. J. B, 86, (2013) 435.
[11] I. O. Troyanchuk, D. V. Karpinsky, M. V. Bushinsky, V.
Sikolenko, V. Efimov, and A. Cervellino, JETP Lett.,
93, (2011) 139.
[12] R. Oishi-Tomiyasu, M. Yonemura, T. Morishima, A.
Hoshikawa, S. Torii, T. Ishigaki, and T. Kamiyama, J.
Appl. Crystallogr., 45, (2012) 299.
[13] J. RodrÌguez-Carvajal, Physica B (Amsterdam,
Neth.), 192, (1993) 55.
[14] A. Wills, Physica B (Amsterdam, Neth.), 278, (2000)
680.
[15] Devendra Kumar and A Banerjee, J. Phys.: Condens.
Matter, 25, (2013) 216005.

Z. Tan1, P. Miao1, M. Hagihala1,2, S. Torii1,2, and T. Kamiyama1, 2Institute of Materials Structure Science, KEK; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center

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Research and Development Highlights

Crystal Structure, Ionic Conductivity and Li-Ion Diffusion
Pathway in a La-Li-Co-O System
1. Introduction
The development of lithium (Li)-ion batteries is being driven by an ever-increasing demand to shift fromfossil fuels to electricity, along with the use of more renewable energy on the grid. Enhancing the energy storage capacity remains a central objective of research on
cathode, electrolyte and anode materials. For example,
our previous study revealed a pronounced influence ofthe type of electrolyte on the capacity [1, 2].
Progress in the field of oxide electrolytes has been
severely hampered due to the lack of new families ofcandidate compounds besides the classic d0 and themain-group element systems (for example, Ti4, Ge4and Zr4) [3–5]. On the other hand, cobalt oxides haveattracted great interest in recent years because of theobservations of huge thermoelectric power [6], superconductivity [7] and a variety of peculiar physical properties reported by our group [8–11], which are generally
considered to be associated with the valence state andthe spin state of Co ions.
2. Experiments
Polycrystalline La-Li-Co-O samples were prepared by solid-state reaction. The details of the crystal
structure analysis, sample characterization and ionic/
electronic conductivity measurements were reported
elsewhere [12]. The neutron time-of-flight diffraction
data at room temperature and 100°C were obtained using a high-resolution neutron powder diffractometerat the BL09 (SPICA) beamline in the Materials and Life
Science Experimental Facility (MLF) of J-PARC, Japan.
The structural parameters were refined using the
Z-Rietveld program [13, 14]. The maximum entropy
method (MEM) calculations were performed using the
Z-MEM algorithm in the Z-code software package [15].
The crystal structure and nuclear density distribution
were visualized using the VESTA program [16].
3. Results and discussion
Li intercalation was performed on parent La2Li0.5Co0.5O4
with tuning x and y in La4/3xLi3xy☐2/3Li0.5Co0.5O4. The chemically fabricated materials exhibited electronic insulating
and ionic conducting behavior. La1.24☐2/3Li0.73Li0.5Co0.5O3.23(x  0.09, y  0.46,   0.77) exhibited the highest Li-ion
conductivity (7 105 S cm1 at 140°C) among all preparedsamples.

The structural analysis carried out for the La-LiCo-O system was the Rietveld refinement for the neutron diffraction profile. Figure 1(a) shows the neuron
diffraction pattern of La1.24☐2/3Li0.73Li0.5Co0.5O3.23. The
orthorhombic Ammm (No. 65) symmetry was applied
and the intercalated Li ions were located at (0, 0, 0.25).
The Li atoms together with vacancies were distributedin the interstitial sites. The lattice was refined as a 
5.35 Å, b  5.35 Å and c  12.62 Å, with RWP  7.94%. The
crystal structure of La1.24☐2/3Li0.73Li0.5Co0.5O3.23 is shownin Fig. 1(b). The MEM was applied to determine the precise nuclear densities. The Li nuclear density was indistinctly localized at room temperature (Fig. 2(a)). Whenthe temperature was increased to 100°C, Li cations diffused throughout a quasi-one-dimensional (Q1D) pathway along the b–axis direction via exchange between
interstitial Li and vacancies (Fig. 2(b)). An increase in thenumber of the Q1D pathway and/or the dimensionalityof the pathway (i.e., isotropic diffusion) is desirable forrealizing higher Li-ion conductivities.

(a)

(b)

Figure 1. Structural characterization of La-Li-Co-O. (a) Neutron
powder diffraction pattern of La1.24☐2/3Li0.73Li0.5Co0.5O3.23
and (b) its crystal structure.

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Research and Development Highlights

MLF Annual Report 2018

(a)

(b)

Figure 2. Nuclear density distribution at z≈0.25 calculated using the MEM with the neutron powder diffraction
data at (a) room temperature and (b) 100°C for La1.24☐2/3Li0.73Li0.5Co0.5O3.23.

4. Conclusion
We discovered the La-Li-Co-O electrolyte as a leading contender. We applied the MEM to the neutron diffraction data. The MEM is expected to be effective for 3D
visualization of diffusional pathways of other cations/anions in next-generation batteries such as sodium-ion
batteries and fluoride-ion batteries, which currently is
being developed.
References[1] T. Takami et al., J. Alloys Compd. 769, 539 (2018).
[2] T. Takami et al., AIP Advances 9, 045301 (2019).
[3] U. v. Alpen et al., Electrochimica Acta 23, 1395
(1978).
[4] C. Wang et al., J. Electrochem. Soc. 151, A1196(2004).
[5] H. Buschmann et al., Phys. Chem. Chem. Phys. 13,
19378 (2011).
[6] I. Terasaki et al., Phys. Rev. B 56, R12685 (1997).

[7] K. Takada et al., Nature 422, 53 (2003).
[8] T. Takami, Functional Cobalt Oxides: Funda mentals, Properties and Applications; Pan Stanford,(2014).
[9] T. Takami et al., Phys. Rev. B 76, 144116 (2007).
[10] T. Takami et al., Appl. Phys. Lett. 99, 072102 (2011).
[11] T. Takami et al., Appl. Phys. Lett. 101, 102409 (2012).
[12] T. Takami et al., ACS Applied Energy Materials 1,
2546 (2018).
[13] R. Oishi et al., Nucl. Instrum. Methods Phys. Res.,
Sect. A 600, 94 (2009).
[14] R. Oishi-Tomiyasu et al., J. Appl. Crystallogr. 45, 299(2012).
[15] Y. Ishikawa et al., ICANS XXI: International
Collaboration on Advanced Neutron Sources,
DAA-P08; J-PARC: Tokai, Japan, (2014).
[16] K. Momma and F. Izumi, J. Appl. Crystallogr. 41, 653(2008).

T. Takami1, Y. Morita1, M. Yonemura2,3, Y. Ishikawa2,3, S. Tanaka4, M. Mori4, T. Fukunaga1, and E. Matsubara1
Oﬃce of Society-Academia Collaboration for Innovation, Kyoto University; 2Neutron Science Section, Materials and Life Science Division,
J-PARC Center; 3Institute of Materials Structure Science, KEK; 4Research Institute of Electrochemical Energy (RIECEN), National Institute ofAdvanced Industrial Science and Technology (AIST)

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MLF Annual Report 2018

Research and Development Highlights

High-Speed Neutron Imaging Using a Current-Biased
Delay-Line Detector of Kinetic Inductance
1. Introduction
Recent progress in the development of intensive
neutron sources and the required peripheral equipment has allowed us to perform simultaneously energyresolved and high-spatial-resolution neutron imaging
and tomography [1]. Much effort has been devoted
to developing a neutron imager with high spatial andtemporal resolution. Recent shortage of 3He isotope,
which is widely used as neutron absorber in neutron
detectors, has also motivated the development of 3Hefree neutron detector.
The highest spatial resolution of 2 m was achievedby a gadolinium-oxysulfide-scintillator camera detector with a reactor neutron source [2]. The scintillation
light was magnified by an optical microscope and wasimaged by a cooled sCMOS camera. To obtain a highspatial resolution image, the center-of-gravity corrections were applied to refine the scintillation-event positions. A 10B-doped multichannel plate (MCP) combinedwith a Timepix readout was also investigated as a neutron imager for pulsed neutron sources [3, 4]. The spatial resolution was 55 m and was improved down to
10 m by using center-of-gravity corrections, while thedetection-rate tolerance decreased due to the computational time.
We have been developing a 3He free all solid-state(a)neutron detector with high spatial and temporal resolution based on a superconducting detector [5–7]. Ourdeveloped system, a current biased kinetic inductance detector (CB-KID), can work as a neutron imager,
while the detector should be cooled down to below
superconducting transition temperature with sub-mA
DC bias currents. We employ the delay-line method to
obtain two-dimensional images with limited readoutlines [7].
2. Detector structure and principle
Figures 1(a) and (b) show the schematic of our delay-line CB-KID system and cross-sectional image of thedetector. Both the X and Y superconducting Nb striplines of 1 m width are folded to meanderlines by every
segment length of h  10.5 mm with a spacing of 1 m.
The X and Y meanderlines are orthogonal to each other,and fabricated on a Nb ground plane. An enriched-10B
neutron-absorption layer is superimposed on top of thedetector. The Nb meanderline with two end electrodes
was fabricated in the Clean Room for Analog-DigitalSuperconductivity (CRAVITY) at the National Instituteof Advanced Industrial Science and Technology (AIST).
The 10B layer was deposited using a molecular beamtechnique under ultrahigh vacuum at Osaka Prefecture
University.

(b)h = 10.5 mm- Ch3

Si substrate SiO2
10

B

y

Y axisIb+ Ch4
x meanderline
y meanderline
Nb ground plane

10

B Layer
x

Ib

- Ch1
+ Ch2

X axisFigure 1. (a) Schematic of the CB-KID system. An X meander is orthogonal to a Y meander. The 10B conversion
layer is deposited on the CB-KID system. Bias currents Ibx and Iby are fed to the X and Y meandelines
independently. Both ends of the two meanderlines are connected to the channels, Ch1, Ch2, Ch3
and Ch4, of a Kalliope-dc readout circuit. (b) Schematic cross-sectional image of CB-KID system.

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Research and Development Highlights

MLF Annual Report 2018

An incident neutron creates charged particles by
the 10B  n reaction at the neutron-absorption layer.
The emitting charged particle to meanderlines induces
rapid reduction of Cooper pair density ns locally at a hot
spot within a tiny segment of the meanderlines. Then, atransient change in the kinetic inductance Lk occurs, because Lk of a superconductor is a function of ns. The voltage pulse across the hot spot arises from the transientchange in Lk under DC bias current. The signals propagate as the electromagnetic waves along the meanderline toward the both ends with opposite polarity. In thepresent work, Ch1 and Ch2 (Ch3 and Ch4) were used
for the collection of signals from the Y (X) meanderline.
We assume that the neutron incident event occurs
at a certain elapsed time t0 from the reference time, andthen t0 can be estimated as1
l  1
l
t0  2  tCh3  tCh4  v   2  tCh1  tCh2  v  ,xywhere tCh1, tCh2, tCh3, and tCh4 are the time stamps of thesignals received at Ch1, Ch2, Ch3, and Ch4, respectively.
l (52.5 m) is the total length of the meanderline, andvx ( 9.04 107 m/s) and vy ( 7.24 107 m/s) are thepropagation velocities for the x and y meanderlines,
respectively. It is noteworthy that one can determine
t0 from the combination of tCh1and tCh2, or tCh3 and tCh4,
independently. If the signals originate from the same
event, t0 in X and Y meanderlines should coincide witheach other. We can identify a genuine combination of asignal quartet by using this coincidence criterion, even
if several signals exist simultaneously on a meanderline.
Therefore, a CB-KID has a good multi-hit tolerance. The
neutron incident position X and Y is determined as
t v
X  ceil  x x  p,2h 

tx  tCh4  tCh3,

t v
Y  ceil  y y  p,2h 

ty  tCh2  tCh1,

where p is the repetition pitch for the meanderline.
The sensitivity of the CB-KID to -rays is negligibly
small because of the low absorption probability of theconstituent materials and the small effective thicknessof the Nb meanderline for  -rays.
3. Experimental method
Our neutron detector is cooled down to 4 K by using a Gifford-McMahon refrigerator. The mechanical vibration of the system is suppressed by an antivibration
cryostat.
The signals are amplified and detected by a Kalliopedc readout circuit, which has a 1-ns sampling multichannel time-to-digital converter (TDC). The Kalliope circuit
16

was originally developed by Kojima et al. for muon-spin
relaxation measurements [8]. We extend the time window from 64 s to 4.2 s by increasing the bit width of
the TDC from 16 to 32 bits. Thanks to this modification,
the time-stamp measurements of 1-ns temporal resolution over a time window up to 4.2 s are possible without
any dead time before and after data acquisition.
The neutron irradiation experiments were performed at BL10 of the Material and Life Science
Experimental Facility (MLF), J-PARC [9] with the collimator ratio L/D  14 m/0.1 m  140 at 200 kW beam power.
The energy resolution is achieved by the time-of-flight(TOF) method with 33 s full width at half maximum at
10 meV.
4. Neutron transmission Image
Signal width of CB-KID is typically a few tens of ns.
It implies the detection-rate tolerance to be as high asa few tens of MHz because CB-KID can handle multi-hit
events. This relatively high detection-rate tolerance of
CB-KID allows high-speed measurements and energydispersive neutron imaging with the combination of
the TOF technique in a pulsed neutron source.
We conducted a neutron-imaging demonstrationby using a well-shaped neutron absorber as a test pattern. The test absorber comprised a 50 m-thick stainless-steel mesh, wherein 100 m 100 m square holes
were arrayed in a square lattice (with a lattice constantof 250 m). Each hole was tightly filled by very fine 10B
particles. We show the neutron transmission image ofthe test pattern in Fig. 2(a). Measurements were performed at T  4.15 K for 30.4 h with an incident neutron
wavelength  ranging 0.05–1.13 nm. The hole size andrepetition period were in a fairly good agreement withthose in the test pattern. The spatial resolutions were
estimated from the sharpness of the dot boundary as
22 m and 41 m in the y and x directions, respectively.
This variance was consistent with that in propagation
velocities. We note that the origin of the error was partially due to the rounding of the etched edges of theholes in the metal mesh.
Figures 2(b)–(e) present the neutron transmission
images of the test pattern corresponding to each with the width of /  1%. Figure 2(b), which has
the image for the   0.05 nm slice, exhibits an unclear
pattern of the test mask. This observation is consistent
with the fact that the 10B neutron-absorption cross-section becomes lower at shorter wavelengths. As shownin Figs. 2(c)–(e), we obtained successfully clear energy
resolved neutron images.

MLF Annual Report 2018

(b)

(c)

(d)

(e)

Research and Development Highlights(a)Figure 2. Neutron transmission images of the 10B dot array contained in the stainless-steel mesh. Neutrons with the wavelength λranging (a) 0.05–1.13 nm, (b) 0.0495–0.0505 nm, (c) 0.297–0.303 nm, (d) 0.693–0.707 nm, and (e) 1.08–1.111 nm are used
to construct the images.

5. Summary
We demonstrated the development of a highspeed neutron imaging system with capability suited
for TOF method. We developed a set of analog signal
discriminators from the preset threshold levels using
a time-to-digital converter with 1 ns resolution over atime frame of 4.2 s. We reconstructed successfully theneutron image of a test pattern with a spatial resolutionof 22 m and the energy-resolved image was producedby the TOF method of pulsed neutrons.
References[1] N. Kardjilov et al., Mater. Today 14, 248 (2011).
[2] D. S. Hussey, J. M. LaManna, E. Baltic, and D. L.

Jacobson, Nuclear Instrum. Methods Phys. Res. A
866, 9 (2017).
[3] A. S. Tremsin et al., Sci. Rep. 7, 40759 (2017).
[4] X. Llopart et al., Nucl. Instrum. Methods Phys. Res. A
581, 485 (2007).
[5] H. Shishido et al., Appl. Phys. Lett. 107, 232601(2015).
[6] S. Miyajima et al., Nucl. Instrum. Methods Phys. Res.
A 842, 71 (2017).
[7] H. Shishido et al., Phys. Rev. Appllied 10, 044044(2018).
[8] K. Kojima et al., J. Phys.: Conf. Ser. 551, 012063 (2014)[9] K. Oikawa et al., Nucl. Instrum. Methods Phys. Res. A
589, 310 (2008)

H. Shishido1,2, T. D. Vu3, K. M. Kojima4,5, T. Koyama5, K. Oikawa6, M. Harada6, S. Miyajima7, M. Hidaka8, T. Oku3, K. Soyama9, K.
Aizawa3, S. Y. Suzuki10, M. M. Tanaka11, and T. Ishida1,2,5
1Department of Physics and Electronics, Graduate School of Engineering, Osaka Prefecture University; 2NanoSquare Research Institute,
Osaka Prefecture University; 3Technology Development Section, Materials and Life Science Division, J-PARC Center; 4Centre for Molecular
and Materials Science, TRIUMF and Stewart Blusson Quantum Matter Institute, University of British Columbia; 5Division of Quantum
and Radiation Engineering, Osaka Prefecture University; 6Neutron Science Section, Materials and Life Science Division, J-PARC Center;
7
Advanced ICT Research Institute, National Institute of Information and Communications Technology; 8Advanced Industrial Science andTechnology; 9Materials and Life Science Division, J-PARC Center; 10Computing Research Center, Applied Research Laboratory, KEK;
11
Institute of Particle and Nuclear Studies, KEK

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MLF Annual Report 2018

Symmetrization of Hydrogen Bond in δ-AlOOH under
Earth’s Mantle Condition
1. Introduction
The study of hydrogen bond under high pressure isimportant to understand the mineral physics under the
Earth’s mantle conditions. In general, hydrogen takes anasymmetric position between two neighboring oxygen
atoms, which forms a long and relatively weak hydrogen bond on one side and a short and strong covalentbond on the other side. However, pressure changes thisasymmetric geometry. It has been theoretically predicted that under high pressure, hydrogen re-locates at thecenter between two oxygen atoms. This phenomenon
is called symmetrization of the hydrogen bond [e.g. 1].
Neutron diffraction is a powerful tool to investigate theposition of hydrogen atom in the structure, however, so
far the study on the symmetrization has been limited toindirect methods such as spectroscopic methods and
X-ray diffraction studies.
In this study, we intended to observe directly thesymmetrization in aluminous hydroxide phase -AlOOH
using neutron diffraction [2]. This phase was foundto be stable at extremely wide pressure range, above
134 GPa and 2000 K, thus it is an important candidateof water carrier into the Earth’s core-mantle boundary
at 2900 km depth.
2. High pressure experiment at PLANET
In this study we measured neutron diffraction on AlOOH and its deuteride under high pressure at PLANET
in MLF [3]. High pressure experiments were conductedusing Paris-Edinburgh cell. Powder sample was sealedin TiZr encapsulating gaskets together with deuterated methanol-ethanol mixture, which maintains thequasi-hydrostatic condition. Diffraction patterns werecollected for 4–7.5 h at several oil pressures upon compression. The obtained profiles were fitted by means of
Rietveld method to refine the atomic positions including hydrogen.
3. Results and discussion
The diffraction profiles were successfully collected
up to 18.1 GPa for -AlOOH and up to 17.4 GPa for AlOOD (Fig. 1). Previous studies have determined the
crystal structure at ambient pressure to be distorted
rutile type with space group of P21nm. In this model,
the AlO6 octahedra make a single chain along c-axis andhydrogen bond is formed in the tunnel between the
chains (Fig. 2(a)). The refinement was conducted using
this model in the first step.
As pressure increased, we observed importantfeatures that indicate a phase transition. First, the difference of the interatomic distance of Al-O1 and Al-O2
atoms of AlO6 octahedra becomes negligible at highpressure. This reflects the fact that two oxygen atoms,
one of which is a donor and the other an accepter ofhydrogen bond, become electrostatically equivalent.
In addition, the intensity of 021 reflection around 1.7 Å
continuously decreases at high pressure. The extrapolation of pressure evolution of the intensity of 120 showsthat it disappears at 9 GPa. This additional extinction
condition can be explained by the phase transition to

Figure 1. Neutron diffraction pattern of δ-AlOOH obtained at 18.1 GPa. The crosses, red andgray lines represent observed, calculated, and difference profiles, respectively.

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MLF Annual Report 2018

Research and Development Highlights

Figure 2. (a) Crystal structure of aluminous hydroxide δ-AlOOH at ambient pressure. (b, c) Change of nuclear density
at high pressure obtained by neutron diffraction. The maps are enlarged around the hydrogen atom (pinkspheres in (a)) and hydrogen is recognized as a negative (blue) peak. (d) Schematic diagram of the change of
proton potential towards hydrogen bond symmetrization at high pressure.

Pnnm, which is a direct super group of P21nm.
The present study indicates that there is a phasetransition in -AlOOH at 9 GPa, however, whether thisrelates to the symmetrization or not is still unclear. To
investigate the hydrogen bond configuration precisely, the difference Fourier map was investigated. In the
Fourier map, the hydrogen atom appears as a negative
peak since it has a negative scattering length for neutron. At the transition pressure, nuclear density displays
bimodal distribution around the center between two
oxygen atoms (Fig. 2(b)). This result implies that thetransition at 9 GPa originates from a disordering of hydrogen bond rather than the symmetrization. Further
compression to 18.1 GPa results in the unimodal distribution, suggesting that the symmetrization wasachieved at this pressure (Fig. 2(c)). The O...O distancereaches 2.41 Å at 18.1 GPa, which agrees with the theoretical prediction. It was fond that the deuterization of
the sample led to an increase of the disorder pressure to
12 GPa. At up to 17.4 GPa, the deuterium atom remains
in a disordered state and the symmetrization seems tooccur at higher pressure.
Comparing the present result and previous studies, a link between the hydrogen bond symmetrizationand the change of physical properties can be discussed.
Previous X-ray diffraction studies have found stiffening behaviors along the a and b axes, where hydrogenbond lies in at around 10 GPa. Brillion scattering experiment also found anomalous increase in sound velocities in the pressure range of 6 to 15 GPa. The present
study indicates that disorder of hydrogen induces these
phenomena rather than the symmetrization.
4. Conclusion
Using neutron diffraction experiments, we observed for the first time that the hydrogen bondsymmetrization occurs in aluminous hydrous phase AlOOH. The results show that changes in physical properties of -AlOOH that had been reported previously
can be explained by the symmetrization and its precursor phenomena of disorder of the hydrogen bond.
References[1] Tsuchiya et al., Geophys. Res. Lett., 29 1909 (2002).
[2] A. Sano-Furukawa et al., Sci. Rep. 8 15520 (2018).
[3] T. Hattori et al., Nucl. Inst. Methods Phys. Res. A, 780
55–67 (2015).

A. Sano-Furukawa1, T. Hattori1, K. Komatsu2, H. Kagi2, and T. Nagai3
Neutron Science Section, Material and Life Science Division, J-PARC Center; 2Geochemical Research Center, The University of Tokyo;
3Department of Earth and Planetary Science, Hokkaido University

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MLF Annual Report 2018

Neutron Spin Resonance in the 112-Type Iron-Based
Superconductor*
1. Introduction
In unconventional superconductors, the neutron
spin resonance mode is a crucial evidence for spin fluctuation mediated superconductivity in the proximity ofan antiferromagnetic (AF) instability [1]. Although thespin resonance mode is theoretically believed to be aspin-1 exciton from the singlet-triplet excitations of
the electron Cooper pairs in copper oxides and heavy
fermions [2], solid proofs of its presence in iron-based
superconductors (FeSC) is still rare. The proximity of superconductivity and AF order, together with the spinorbit coupling (SOC) effect, add more complexity to theenergy and momentum distribution of spin resonance.
In order to seek for a convincing mechanism of high-Tc
superconductivity, it is necessary to study the neutron
spin resonance in more materials [3].

3. Results
A neutron spin resonance mode around ER  11 meV
was discovered for the first time in 112-type FeSC
(Fig. 2) [6]. The resonance mode was almost two-dimensional, and the resonance energy was demonstrated to be almost temperature independent and could
scale with Tc linearly (Fig. 3 and Fig. 4) [6]. Polarized
neutron analysis revealed that the resonance mode
was nearly isotropic in spin space (Fig. 3(c)). Because of
the unique monoclinic structure with additional zigzag
arsenic chains, the As 4p orbitals contribute to a three
dimensional hole pocket around the point and an extra electron pocket at the X point. Our results suggestthat the energy and momentum distribution of the spinresonance does not directly respond to the kz dependence of the fermiology, and the spin resonance intrinsically is a spin-1 mode from singlet-triplet excitationsof the Cooper pairs in the case of weak spin-orbital
coupling [6].

2. Experiments
We have prepared high quality single crystals of the
newly discovered 112-type iron pnictide using the self-flux
method [4, 5] and co-aligned 2.3 g Ca0.82La0.18Fe0.96Ni0.04As2(Tc  22 K, see Fig. 1) single crystals (about 1500 pieces)with a small mosaic about 4° in the ab plane and 3° along
the c axis. By using inelastic neutron scattering, we havecomprehensively studied the low-energy spin excitations of this new 112-type FeSC [6].

* This work has been published on Physical Review
Letters [6]. The neutron-scattering experiment at HRC
was performed with the J-PARC under user proposal
program (2016B0068).

(a)
(b)

Figure 1. (a) Crystal and magnetic structure of the Ca1−xLaxFeAs2 system; (b) Superconducting transitions of Ca0.82La0.18Fe0.96Ni0.04As2.

20

MLF Annual Report 2018

Research and Development Highlights

Figure 2. Neutron spin resonance mode around 11 meV in Ca0.82La0.18Fe0.96Ni0.04As2. (Results from HRC-BL 12)

Figure 3. Two-dimensional, isotropic spin resonance in Ca0.82La0.18Fe0.96Ni0.04As2.

Figure 4. Linear scaling of spin resonance energy ER and superconducting transition temperature Tc in FeSC.

References[1] P. Dai, Rev. Mod. Phys. 87, 855 (2015).
[2] M. Eschrig, Adv. Phys. 55, 47 (2006).
[3] P.D. Johnson, G. Xu, and W.-G. Yin Iron-Based
Superconductivity (Springer, New York, 2015).
[4] N. Katayama et al., J. Phys. Soc. Jpn. 82, 123702(2013).
[5] T. Xie et al.,Supercond.Sci. Technol. 30, 095002(2017).
[6] T. Xie et al., Phys. Rev. Lett. 120, 137001 (2018).

T. Xie1, D.L. Gong1, H. Ghosh2, A. Ghosh2, M. Soda3, T. Masuda3, S. Itoh4,5, F. Bourdarot6, L-P. Regnault7, S. Danilkin8, S.L. Li1,
and H.Q. Luo1
1
Institute of Physics, Chinese Academy of Science; 2HomiBhabha National Institute, AnushaktiNagar; 3The Institute for Solid State Physics,
The University of Tokyo; 4Institute of Materials Structure Science,KEK; 5Neutron Science Section, Materials and Life Science Division, J-PARC
Center; 6Université Grenoble Alpes, CEA; 7Intitut Laue Langevin; 8Australian Centre for Neutron Scattering, Australian Nuclear Science andTechnology Organization

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Research and Development Highlights

MLF Annual Report 2018

Observation of Pressure-Tuned Molecular Reorientational
Dynamics in Barocaloric Neopentylglycol
1. Introduction
Caloric effects are phase-transition thermal effects
regulated by external fields. As a promising alternative to the vapor compression cycle technology that iscurrently in wide service, emerging refrigeration technologies based on solid-state caloric effects have been
attracting attention in recent decades. Large isothermal
entropy changes and adiabatic temperature changes
are the most important requirements for a caloric material. Current caloric materials are characteristic ofsmall isothermal entropy changes of about 50 J kg1K1,which is one of serious obstacles to the real applications. Very recently, we have discovered that plastic
crystals exhibit excellent barocaloric effects with typicalentropy changes higher than 400 J kg1K1 induced bya small pressure,  20 MPa, as shown in Fig.1 [1]. Whilethese findings imply the solid-state refrigeration technologies based on caloric materials would be on thehorizon, the underlying microscopic scenario on suchcolossal barocaloric effects has to be established, as far
as the fundamental issue is concerned.
2. Experimental considerations
As plastic crystals are also called orientation-disordered crystals, the reorientational dynamics mightplay a decisive role in the colossal barocaloric effects. Thus, in-situ high-resolution inelastic neutron
scattering (INS) as well as quasi-elastic neutron scattering (QENS) measurements are proposed on the
representative plastic crystal neopentylglycol (NPG),
whose chemical formula is C5H12O2 and IUPAC name is

2,2-dimethyl-1,3-propanediol.
The cold neutron disk chopper spectrometer BL14
AMATERAS of MLF was chosen for such a study for its
superior energy resolution in wide energy bands accommodated with the multi-Ei capacity [2]. A powder
sample of around 0.29 g was wrapped with aluminium
foil and further sealed into an aluminium can with indium wire. Such a geometry ensures about 80% transmission of neutrons, which is crucial for obtaining
high-quality QENS data. A cryostat was used to access abroad temperature region. The chopper configurations
were 300 Hz (CH01), 300 Hz (CH02) with a slit width of
10 mm, and 150 Hz (CH03), which enabled the selection of Ei  23.72, 5.93, 2.64 meV with energy resolutionof 0.42, 0.078, and 0.026 meV, respectively. The data
reduction was performed using the Utsusemi suite [3].
The resulting S(Q, E) data were visualized in Mslice of
DAVE [4].
The high-pressure INS/QENS data were collectedwith the same Ei but with a slit size of 30 mm to enhance the intensity, using a clamped cell made of an
Al–Zn–Mg-based alloy (Mesoalite). The powder sample was mixed with reagent-grade KBr powder (Kanto
Chemical) to reduce multiple scattering and to ensure
quasi-hydrostatic conditions. We note that KBr has very
limited incoherent scattering length, which is very important for QENS measurements. A mixture of the sample and KBr powder at a volumetric ratio of 1:1 was used
to fabricate a pellet of 6.5 mm diameter and 22.5 mm
length, which was inserted into a sample cell made ofTeflon. The sample was compressed to the desirable

Figure 1. Absolute values of maximum entropy changes, |ΔSmax|, for leading caloric materials. MCE, magentocaloric effect;
ECE, electrocaloric effect; eCE, elastocaloric effect; and BCE, barocaloric effect.

22

MLF Annual Report 2018loading with a hand press, using a load–pressure curve
determined beforehand. The actual pressure generated
in the cell was determined at the high-pressure neutron
diffractometer (PLANET) [5] from the change of the lattice parameters of KBr using the equation of state [6].
3. Results and discussion
The molecular configuration of NPG is characteristic of a tetrahedral motif. The five carbon atoms form atetrahedron, in which two carbon atoms are attachedto hydrogen atoms in the methyl group, whereas twoothers form the hydroxymethyl group. At room temperature, the NPG molecules are ordered on a monoclinic lattice with space group P21/n. This ordered phasetransforms into an fcc lattice at Tt  314 K on heating
under the ambient pressure.
We performed QENS measurements on NPG at selected temperatures near Tt. Shown in Fig. 2(a) are thecontour plots of the dynamic structure factor S(Q, E) as
a function of momentum transfer (Q) and energy transfer (E) with Ei  2.64 meV. The intense stripes centered at
E  0 represent the elastic line, which contains most of
the scattering intensity. It can be seen that the elastic
lines dominate the spectra at 250 K and 300 K. At 320 K,
just above Tt, a less-intense signal spreads out from E  0
and weakens as E increases, which corresponds to QENS(a)

Research and Development Highlights

originating from hydrogen atoms. The spectra fitting
suggests that the hydrogen atoms in the methyl groupare subjected to C3 reorientation in both ordered anddisordered phases (C3 reorientation might be further
frozen at about 60 K), while the whole molecule undergoes isotropic reorientation in the disordered phase.
More strikingly, the pressure-dependent QENS
data directly provide insights into the microscopic dynamics of the system. It can be seen in Fig. 2(b), (c) that
the QENS signal, which appears as a trail of the intense
elastic line, is mostly suppressed under a pressure of
286 MPa. Indeed, the QENS intensity is already effectively suppressed even at a lower pressure of 178 MPa.
These QENS data directly verify that orientational disorder is restrained by the pressure, inducing entropychanges. The pressure suppression of orientational disorder is also manifested in phonons. Shown in Fig. 2(d),(e) are S(Q, E) with Ei  23.72 meV at ambient pressure
and at 286 MPa, respectively. It is clear that the phonons
centered at about 4 meV become considerably sharperat 286 MPa, which is attributed to the reduced scattering by the orientational disorder. These experimental
insights unambiguously indicate that the colossal barocaloric effects of NPG can be attributed to the suppression of the extensive orientational disorder by pressure.

(b)

(d)

(c)

(e)

Figure 2. (a), Contour plots of S(Q, E) at five temperatures around Tt, obtained with Ei = 2.64 meV at AMATERAS. (b), (c), QENS measurements at ambient pressure and 286 MPa obtained at 325 K with Ei = 2.64 meV. (d), (e), INS measurements at ambientpressure and 286 MPa obtained at 325 K with Ei = 23.72 meV. We note that the inelastic signals at about 1.3, 2.6, 4.4 and5.1 Å−1 are contributed by phonons from Teflon.

23

Research and Development Highlights

MLF Annual Report 2018

4. Prospect
The core physical issue of caloric materials is theevolutions of atomic structures and interactions as afunction of driving forces including pressure, magnetic
fields, electric fields, stresses as well as light illuminationin multiple spatial and temporal scales. State-of-the-art
characterization techniques based on large-scale facilities such as the neutron scattering are highly desirable
in this case due to the powerful experimental abilities
and versatile complex sample environments. In otherwords, the experimental techniques based on largescale facilities provide a great opportunity for caloric
materials research and we hope that our present study

would inspire both the neutron scattering and caloric
materials communities.
References[1] B. Li et. al., Nature, 567 506 (2019).
[2] K. Nakajima, et. al., J. Phys. Soc. Jpn, 80 SB028(2011).
[3] Y. Inamura et. al., J. Phys. Soc. Jpn 82 SA031 (2013).
[4] R. T. Azuah et. al., J. Res. Natl. Inst. Stand. Technol.
114 341–358 (2009).
[5] T. Hattori et. al., Nucl. Instrum. Methods Phys. Res. A
780 55–67 (2015).
[6] A. Dewaele et. al., Phys. Rev. B 85 214105 (2012).

B. Li1, Y. Kawakita2, S. Ohira-Kawamura2, T. Hattori2, T. Kikuchi2, Z. Zhang1, Z. Zhang1, W. J. Ren1, Z. D. Zhang1, and K. Nakajima2
Shenyang National Laboratory for Materials Science, Institute of Metal Research CAS; 2Neutron Science Section, Materials and Life Science
Division, J-PARC Center

1

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MLF Annual Report 2018

Research and Development Highlights

A New Method for Structural Analysis of a SpecificProtein or Lipid Membrane in a Molecular-Crowding
Environment Mimicking Living Cells
1. Introduction
The interior of the living cells is a molecular-crowding environment wherein numerous molecules coexist
at about 30–40% v/v. The structural stability of proteinsin aqueous solutions is well known to vary by the presence of co-solutes (osmolytes) such as sugars andpolyols. Thus, the equilibrium states of biological macromolecular systems are affected by molecular-crowding
environments unmatched by in vitro diluted environments. In particular, molecular-crowding environments
affect the interaction energy between the water layers
and proteins and alter the hydration structure and accessible volume depending on protein size via changes
in chemical potential and activity. However, the theoretical interpretations of the molecular-crowding effectin living cells remain controversial, as it is difficult to predict with certainty the behavior of a specific molecule.
On the other hand, by the combination of neutronand synchrotron X-ray scattering methods, we clarified
the effect of small or large molecular weight osmolytes(sugar, polyol, and synthetic neutral polymer) on protein structure and its hydration [1–3]. We also reported
that the presence of those molecules affected the structural stability of proteins against chemical and thermal
perturbations [4–6]. However, as various kinds of intermolecular interactions exist in the interior of living cells,
clearly, previous experimental conditions for molecular-crowding do not reflect well the actual environment
inside cells for affording an accurate understanding of
the mechanisms of biological reactions. Hence, oneof the current issues in life science is how to observe
the biological reactions in an environment that closely
mimics the interior of living cells.
Therefore, investigations into the nature of suchan environment are essential to understand both theelaborate biological reactions and the maintenance of
homeostasis occurring therein. However, the knowledge about crowding effects is still insufficient due tothe lack of relevant experimental studies. Recent developments in the techniques of in-cell NMR and largescale molecular dynamics simulation are providing new
insights into the structure and dynamics of biologicalmolecules inside the cells. We have demonstrated successfully a new experimental technique for observing

the structure of a specific protein or membrane in themolecular-crowding environment mimicking actual living cells by using the inverse contrast matching method of neutron scattering [7].
2. Experimental
The protein measured in this study was myoglobin.
The small uni-lamellar vesicles (SUVs) measured werethe mixtures of monosialoganglioside (GM1), cholesterol, and 1,2-dipalmitoyl-sn-glycero-3- phosphocholine(DPPC). These SUVs constitute a lipid raft membranemodel. Gangliosides, major components of glycosphingolipid, are acidic lipids composed of a ceramide linked
to an oligosaccharide chain containing one or moresialic acid residues; they are abundant in central nervous systems. Lipid rafts are dynamic assemblies ofsphingolipids and cholesterol in lipid bilayers that function as platforms for membrane-associated events suchas signal transduction, cell adhesion, and lipid/protein
sorting. E. coli (strain BL21) cells were deuterated by theculture in a deuterated cell growth media. These deuterated cells were disrupted by an ultrasonic irradiation
on ice cooling and used as the crowder for mimicking
environment of living cells. Further in this text, we willcall this crowder cell debris.
The small- and wide-angle neutron scattering(SWANS) measurements were carried out on a BL15TAIKAN spectrometer at the pulsed-neutron sourceof the Materials and Life Science Experimental Facility(MLF) of the Japan Proton Accelerator ResearchComplex (J-PARC, Tokai, Japan).
3. Results and discussion
At first, we characterized the cell debris in solution
using the dynamic light scattering method (DLS) andthe solvent contrast variation method of neutron scattering (SCV). The average diameter of the cell debris was7.5 nm in number distribution and 1.4 m in intensity
distribution. The size distribution function indicatedthat the crowder solution was rather polydisperse.
Comparing the number distribution function with thatof scattering intensity, showed that the cell debris included large molecules, but still their major components were small molecules and fragments. From the25

Research and Development Highlights

MLF Annual Report 2018

small-angle neutron scattering (SANS) curves of the celldebris (2% w/v) in the different H2O/D2O mixed solvents(100, 75, 50, 25, and 0% v/v D2O) at 25°C, the contrast
matching point of the cell debris was determined by
97.6% D2O. The Porod plot and the Orstein-Zernike plotof the SANS curve of the cell debris solution (15% w/v in
H2O, at 25°C) indicated that the cell debris solution has
the feature of a diffusion-limited aggregate solution
with a correlation length of 265 Å. In addition, the celldebris solutions did not exhibit any distinct scatteringprofile that might pose an obstacle for data correction.
This is important for extracting structural informationof a specific protein or liposome from the backgroundscattering of the crowder solutions.
Based on the above characterization of the cell-debris solution, we carried out the SWANS measurementsof the protein and the SUVs in cell debris solutions (in97.6% D2O). The protein concentration varied from
0.25% to 5.0% w/v in 15% w/v cell debris. The minimum protein ratio in concentration ([protein] / [celldebris]) was 1/60 w/w. In the case of SUVs, the lipid

concentration was fixed by 0.5% w/v, and the cell debris
concentration was varied from 7% to 21% w/v. After executing a background correction based on the method
appropriate for the wide-angle scattering data [8], wemanaged to determine the structure of the specificprotein or SUV up to the concentration ratio of [protein
or SUV] / [cell debris]  1/60 or 1/40. Figure 1 shows
the photos of the cell debris solutions and the SWANS
curves of the protein in the cell debris solution (15%w/v) [7]. By comparing the observed SWANS curves ofthe protein with the theoretical ones obtained by fitting using CRYSON program [9], we have demonstrated
that the protein structure is determinable even at thelowest concentration (0.25% w/v) in 15% w/v cell debris
solution. The structures of the SUVs have been also determined successfully. It should be noticed that the celldebris crowder used in this experiment can reproduce
an environment that more closely mimics the interior ofliving cells than model crowders used previously suchas polyols and synthetic polymers.
4. Future plans
The present results clearly indicate that not only
the in-cell NMR technique and in silico approaches, butalso the inverse contrast matching method using thedeuterated-cell debris provide a promising technique
for studying the structure and dynamics of biologicalmacromolecules in intracellular molecular-crowding
environments that are essential in controlling biological systems. We are executing further experiments toclarify the specific interaction between a protein andlipid raft membrane.

Figure 1. A, photos of the solutions composed of cell debris.
B, comparison of the observed SWANS curves of
myoglobin (0.25–5% w/v) in 15% w/v cell debris
with theoretical ones obtained by fitting using
CRYSON program.

References[1] S. Ajito, et. al., Physica B: Condensed Matter, 551,
249 (2018).
[2] M. Hirai, et. al., Biophysical J., 115 313 (2018).
[3] M. Hirai, et. al., Physica B: Condensed Matter, 551,
212 (2018).
[4] S. Ajito, et. al., J. Phys. Chem. B, 122, 8685 (2018).
[5] M. Hirai, et. al., J. Phys. Chem. B, 122, 9482 (2018).
[6] M. Hirai, et. al., J. Phys. Chem. B, 122, 11962 (2018).
[7] M. Hirai, et. al., J. Phys. Chem. B, 123, 3189 (2019).
[8] M. Hirai, et. al., Biochemistry, 43, 9036 (2004).
[9] D. I. Svergun, et. al., J. Appl. Cryst., 28, 768 (1995).

M. Hirai1, S. Ajito1, S. Arai2, M. Adachi2, R. Shimizu2, S. Takata3, and H. Iwase4
Graduate School of Science and Technology, Gunma University; 2National Institute for Quantum and Radiological Science and Technology;
3
Netron Science Section, Materials and Life Science Division, J-PARC Center; 4Neutron Science and Technology Center, CROSS

1

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MLF Annual Report 2018

Research and Development Highlights

Directed Diffusion of Photovoltaic Active Layer
Components into Porous ZnO-based Cathode Buffer
Layers in Polymer Solar Cells
1. Introduction
Cathode buffer layers (CBLs) can successfully stretch
further the efficiency of polymer solar cells (PSCs), after
optimization of the active layer. Hidden between theactive layer and the cathode of the inverted PSC device configuration is the critical yet often-unattended
vertical diffusion of the active layer components across
CBL. Here, we develop a novel methodology of contrast
variation with neutron and anomalous X-ray reflectivity(NR and AXR) to map out the multi-component depth
compositions of an inverted PSC, covering the area fromthe active layer surface down to the bottom of the ZnObased CBL. Uniquely revealed for a high-performancemodel PSC are the often-overlooked porosity distribution of the ZnO-based CBL and the differential diffusionsof the polymer PTB7-Th and fullerene-derivative PC71BM
of the active layer into the CBL. Interface modification of
the ZnO-based CBL with fullerene-derivative PCBE-OH
for size-selective nanochannels can further selectively
improve more the diffusion of PC71BM than that of thepolymer. The deeper penetration of PC71BM establishes a gradient distribution of fullerene-derivatives overthe ZnO/PCBE-OH CBL, resulting in markedly improved
electron mobility and device efficiency of the inverted
PSC. The result suggests a new CBL design concept ofprogressive matching of the conduction bands, via directed vertical diffusion of the active-layer fullerenederivatives into porous, fullerene-decorated ZnO-CBLs.
2. New methodology and result
The new contrast methodology, which uses NR and
AXR for revealing the interfacial structures of PSCs, isbased on the changes of the scattering power of themetallic atoms in the metallic oxide of CBL, to neutrons
and X-rays at energies away and close to the absorption
edges of the metallic atoms [1–2]. With the rich andeasy changes in the scattering contrast, the developed
methodology opens a new channel to resolve increasingly complicated interfacial structures and depthcompositions of PSCs with multi-doped, metal-oxide
cathode buffer layers. Here, we show an example thatthe new method can map successfully the multi-component depth compositions of a model PSC with ZnObased cathode buffer layers.

The in-plane averaged density or scattering-lengthdensity profile (z) of a stratified film through the film
thickness can be reconstructed from an XR or NR profile measured as a function of the scattering vector qz( 41sin, with wavelength  and incident angle )
along the film normal [2]. A scattering-length-density(SLD) profile ¯(z) of the film then can be reconstructed from the data. For a n-component system, ¯(z) ni1 fi(z)ρi is contributed by the n components of the corresponding scattering-length-density i, weighted by
the depth-dependent volume fraction fi(z). Therefore,
resolving the fi(z) profiles of the n-component system
requires n sets of ¯(z) profiles reconstructed respectively from n sets of reflectivity profiles measured for thesame film structure, with varied scattering contrasts.
This can be achieved by NR and AXR measurements fora same film, with X-ray energy E tuned near and away
the absorption K-edge of the selected metallic atoms
ρEi (z) values. Thus, the depth-deof the film for varied ¯pendent composition profiles of the film can be solvedby the following relations arranged in a matrix form
ρ1,E1
ρE1(z)¯ρ¯
ρ1,E2
E2 (z)=⋯⋮ρEn(z)
¯
ρ1,En

ρ2,E1
ρ2,E2
⋯
ρ2,En

⋯
⋯
⋯
⋯

ρn,E1
ρn,E2
⋯
ρn,En

f1(z)
f2(z)
⋮
fN(z)

(1)

where ¯ρEi (z) is individually deduced from the model fitting of corresponding anomalous XR data measured
with X-ray energy Ei. For better resolution, NR is used
as one of the relations in the matrix (1) for enhanced
contrast variation. This is because fullerene-derivatives
often used in PSCs have a markedly higher neutron
scattering-density-density ρN than that of the conjugated polymers, thereby, providing a higher scattering
contrast for increased sensitivity to fullerene distribution. In (1), ρn of each neat component can be calculated
or measured from a neat film. We note that summationof fn(z) is less than 1 for a system with porosity [3].
We applied the above methodology to map the
depth composition of a model PSC, comprising theactive layer of conjugated polymer PTB7-Th and C70derivative PC71BM and a ZnO-based CBL selectively
doped with a C60-derivative PCBE-OH [4]. Three sets of27

Research and Development Highlights

MLF Annual Report 2018

anomalous XR profiles measured with the three X-ray
energies of E1  9400 eV, E2  9651 eV, and E3  9656 eV(near the absorption K-edge EK of Zn in ZnO), complemented with one set of NR data, were used to solve thedepth-dependent distributions of the four-component
system from the surface of the PSC active layer down tothe bottom of the CBL.
Shown in Fig. 1(a) are the NR and AXR data for an
active layer of PTB7-Th:PC71BM on a ZnO-C60 CBL, spincoated on Si substrate. These data are jointly fittedusing the ρ̄x (representatively shown for the E2 case)and ¯
ρN profiles shown in Fig. 1(b). With the obtained
four SLD profiles, we then solved depth-by-depth thefour volume fractions on the basis of (1) for the depthdependent composition (volume fraction) profiles fi(z)of the active layers of PTB7-Th: PC71BM (1:1.5, w/w)
on ZnO-C60–doped ZnO CBL, as shown in Fig. 2(a).
Reconstructed from the deduced composition profiles
is the schematics shown in Fig. 2(b) for the vertical distributions of PTB7-Th and PC71BM of the active layers
spin-coated on the ZnO-CBL doped with PCBE-OH.

(a) 3

(b)

E2
E3

-6

-1

log R

6

-2

0

NR

30

-2

NR

ρ X (10 Å )1

8

XR(E2)

-2
-3

20

4

to Air10-4

Active Layer

ZnO-C60-62XR

ρ N (10 Å )

E1

2

-5
0

-6

0

Si substrate

-7
0.05

0.01

0

0.2

0.1

200

-1

qz (Å )

400

600

800 1000 1200

z (Å)

Figure 1. (a) Neutron and anomalous X-ray reflectivity data for an active layer of PTB7-Th:PC71BM on a ZnO-C60 CBL, spin-coated on
Si substrate. Data are jointly fitted (solid curves) using (b) the ρ̄x (representatively shown for the E2 case) and ρ̄N profiles.
For clarity, XR data with E1 and E2 are shifted vertically. The shaded zones in (b) are the transition zone and the ZnO-C60 CBLsitting on Si substrate (z = 0).

0

200

400

600

1200

1.2
1.0

PTB7-Th
PCB71M

0.8

ZnO
PCBE-OH

to Airf (z)Porosity
0.6

ZnO-C60

(b)

PCBM

(a)

≈

90 Å

0.4

Active Layer

0.2
0.0

to Si substrate
0

200

400

600

PCBE -OH

PC 71 BM and Aggregate

ZnO

PTB7- Th and Crystallite

1200

z (Å)
Figure 2. (a) Depth composition (volume fraction) profiles f(z) for the active layers of PTB7-Th: PC71BM (1:1.5, w/w) on ZnO-C60.
Shaded areas highlight the surface and interface transition zones of distinct phase segregations. (b) Schematics for thevertical distributions of PTB7-Th and PC71BM of the active layer spin-coated on the ZnO-based CBLs, with the doped
fullerene-derivative PCBE-OH enriched at the bottom part of the CBL (bridging the pathway for electrons).

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MLF Annual Report 2018

3. Conclusion
We have developed a new methodology on thebasis of contrast variation with neutron and anomalous X-ray reflectivity, which can map successfully themulti-component depth compositions of a model PSC
with ZnO-based cathode buffer layers. The results reveal the differential vertical diffusion behaviors of the
PSC components into the ZnO cathode buffer layer andthe critical yet long-overlooked porosity distributionof the ZnO CBL. The advantages of doping ZnO CBLs
with fullerene-derivatives are illustrated with the modified interfacial structures across the ZnO-fullerene CBL
and the selectively enhanced vertical diffusion of thefullerene-derivatives from the active layer. The hence
established depth-concentration gradient of fullerenederivatives in the ZnO-C60 CBL is associated with the improved electron mobility and device performance; thispositive correlation suggests a new CBL design concept
with progressive matching of conduction bands in inverted PSCs. With neutron reflectivity and synchrotron

Research and Development Highlights

anomalous X-ray reflectivity for rich scattering contrast
variations, the developed methodology opens a newchannel to resolve increasingly complicated interface
structures and depth-compositions of PSCs with multidoped, metal-oxide cathode buffer layers.
4. Instruments
Anomalous X-ray reflectivity measurements werecarried out at Beamline 07 of the Taiwan Light Source(TLS) of the National Synchrotron Radiation ResearchCenter (NSRRC), Hsinchu. Neutron reflectivity measurements were conducted at BL16 SOFIA neutron reflectometer in J-PARC MLF, Japan, with data collected intime-of-flight mode.
References[1] J.-J. Kang, et al. Small 14, 1704310 (2018).
[2] W.-R. Wu et al. Adv. Energy Mater. 7 1601842 (2017).
[3] H.-J. Liu et al. Soft Matter, 7, 9276 (2011).
[4] H. Liao, et al. Adv. Mater. 25, 4766 (2013).

J.-J. Kang1,2, T.-Y. Yang3, Y.-K. Lan4, W.-R. Wu1, C.-J. Su1, S.-C. Weng1, N. L. Yamada5,6, A.-C. Su3, and U- Jeng1,3
1National Synchrotron Radiation Research Center, Taiwan; 2Physik-Department Technische Universität München, Germany; 3Department ofChemical Engineering, National Tsing Hua University, Taiwan; 4National Chung Shan Institute of Science and Technology, Taiwan; 5Neutron
Science Section, Materials and Life Science Division, J-PARC Center; 6Institute of Materials Structure Science, KEK

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Research and Development Highlights

MLF Annual Report 2018

Probing a Unique Spin Texture of 4f Electron Magnet
EuPtSi
1. Introduction
Magnetic skyrmions are particle-like, topologically
non-trivial spin textures that have attracted interest
because of their fundamental aspects as well as applications due to their potential as a low-power-consumption device. The magnetic skyrmion lattice can be
represented by a triple-q magnetic order in which threehelical propagation vectors make an angle of 120° witheach other in the plane normal to the applied field H.
Therefore, the six-fold magnetic pattern in the plane
normal to H in the neutron diffraction is a crucial evidence for a formation of skyrmion lattice. This realization was first identified in a chiral magnet MnSi by thesmall angle neutron scattering [1]. This discovery has
triggered an intensive search for compounds with similar crystal structures, leading to the discovery of their
existence in FeGe [2] and the insulator Cu2OSeO3 [3].
Various characteristic properties have been unveiled
as the number of skyrmion compounds has increased.
Unlike this diversity, magnetic ions have been mostly
limited to 3d transition metal elements.
Recently, high-quality single crystals of the 4f electron compound EuPtSi with a similar crystal structure
have been grown. In EuPtSi, seven 4f electrons carrymagnetism. This compound exhibits an antiferromagnetic transition at TN  4 K at a zero magnetic field [4].
Characteristic features emerged under magnetic fields,
including a field-induced phase, i.e., the A-phase, whichappeared only at a finite temperature and a magnetic

Figure 1. Magnetic phase diagram of EuPtSi for H || [111] [4].
The field-induced A-phase only exists at a finite
temperature and magnetic field.

30

field, as shown in Fig. 1. This feature, common to the skyrmion phase of MnSi, implies the existence of a magnetic
skyrmion in EuPtSi. To obtain microscopic insights into
magnetic ordering phenomena in EuPtSi, single-crystal
neutron diffraction experiments were carried out.
2. ExperimentSingle crystals of EuPtSi were grown by the
Bridgman method using naturally occurring Eu. Several
crystals with typical sizes of 2 2 1 mm3 were used in
the following experiments.
Single crystal neutron diffraction experiments atzero field were carried out on the time-of-flight Lauediffractometer SENJU at BL18 of MLF, J-PARC. A halfpolarized neutron scattering experiment and singlecrystal diffraction experiments under the magnetic
field were carried out on the polarized triple-axis spectrometer HB-1 and the wide-angle neutron diffractometer WAND2, respectively, both installed at the High Flux
Isotope Reactor (HFIR), Oak Ridge National Laboratory(ORNL), U.S.A..
3. Magnetic structure at zero fieldA neutron scattering intensity map of (h, k, 0) recorded at 0.3 K on SENJU is displayed in Fig. 2. In addition to a number of nuclear Bragg peaks with integer
h and k, superlattice reflections with a rectangular pattern were identified around each nuclear peak [5]. The
observed magnetic peaks are characterized by the ordering vector q1  (0.2, 0.3, 0). Note that there is no peakfor q  (0.3, 0.2, 0) even with the cubic structure. The result reveals that the crystal structure is consistent withthe symmetry P213 and the present sample consists ofa single domain.
In order to get further insights into the magnetic
structure with q1, the half-polarized neutron scattering experiments were performed. In case that incoming neutron spins are aligned parallel/antiparallel tothe scattering vector Q (called x channel), the magnetic
peak was observed only for the antiparallel configuration (Ix) as displayed in Fig. 3. A distinct difference between parallel (Ix) and antiparallel (Ix) configurations,and an intense peak only for Ix indicate that Eu magnetic moments form an anti-clockwise helix in the plane
perpendicular to q1, namely, the magnetic structure in
the ground state has a chirality [5].

MLF Annual Report 2018

Research and Development Highlights(1, 0, 1)0.6(h, h, 2h) (r. l. u.)(0, k, 0)

1

2

3

2
(h, 0, 0)

1

+

I

I

x

1.5 K

3

3

Intensity (10 counts / 600 s)(0, 0.2 0.3)

2
0.01

(1, 1, 0)00.5
B || [111]Figure 2. Neutron scattering intensity map of the (h, k, 0)
plane at 0.3 K at zero field [5].

4

0.2

0.2

0.3 K
3

0.4

0
(h, 2h 0.3) (r. l. u.)

0.01

Figure 3. Half-polarized neutron scattering profile of themagnetic reflection (0, −0.2, 0.3) at 1.5 K [5].

4. Magnetic structure in the A-phase
As a next step, the magnetic structure in the fieldinduced A-phase was investigated by single-crystal
neutron scattering experiments for the field appliedalong the [111] direction using the vertical field magnet. In this setup, the horizontal scattering plane is defined by the two orthogonal vectors (H, H, 0) and (H,H, 2H). The magnetic peak of the helical structure q1
does not exist in this horizontal plane. By applying magnetic field of 12 kOe at 1.9 K to enter into the A-phase,the magnetic patterns exhibit substantial change;magnetic peaks emerge in the horizontal scattering
plane and form a six-fold pattern around the nuclear
magnetic peaks, as illustrated in Fig. 4 [5]. The observed
hexagonal peak can be described by the peculiar, threeordering vectors of qA1  (0.09, 0.20, 0.28), qA2  (0.20,
0.28, 0.09) and qA3  (0.28, 0.09, 0.20). Note that these

0

0.5
1.0
(h, h, 0) (r. l. u.)

1.5

Figure 4. Neutron scattering intensity map of the plane normal to the applied field H||[111] recorded in the Aphase [5].

three ordering vectors are equivalent with cyclic permutation and make an angle of 120° with each other.
And the periodic length of qA is the same as q1. These
characteristic features, (i) the three ordering vectors
make an angle of 120° in the plane normal to the applied field, (ii) the same periodicity as in the groundstate helimagnetic structure, are common to the archetypical skyrmion compound MnSi. The present result,
together with the emergence of huge topological Hall
effect, demonstrates a formation of the skyrmion latticein the A-phase of EuPtSi, a first example in the 4f electron magnets [5].
Contrary to the common features mentioned
above, there are distinct differences between EuPtSi
and MnSi. One of the examples is the periodic length.
The periodicity in MnSi is quite long, requiring smallangle neutron scattering to separate magnetic andnuclear peaks, whereas the ‘standard’ diffraction is sufficient to reveal magnetic patterns of EuPtSi owing to
its shorter periodic length: 18 versus 1.8 nm in MnSi and
EuPtSi, respectively. In addition, the A-phase in EuPtSi
was stabilized over a relatively wide temperature range,
whereas that of MnSi exists over only a narrow region inclose proximity to the transition temperature. Overall,
the discovery of a magnetic skyrmion phase in 4f electron systems has provided a new direction to explore
other compounds and has unveiled more characteristics of skyrmions.
References[1] S. Mühlbauer, B. Binz, F. Jonietz, C. Pfleiderer, A.
Rosch, A. Neubauer, R. Georgii, and P. Boni, Science
323, 915 (2009).
31

Research and Development Highlights

MLF Annual Report 2018[2] H. Wilhelm, M. Baenitz, M. Schmidt, U. K. Rößler, A.
A. Leonov, and A. N. Bogdanov, Phys. Rev. Lett. 107,
127203 (2011).
[3] S. Seki, X. Z. Yu, S. Ishiwata, and Y. Tokura, Science
336, 198 (2012).
[4] M. Kakihana, D. Aoki, A. Nakamura, F. Honda, M.
Nakashima, Y. Amako, S. Nakamura, T. Sakakibara,

M. Hedo, T. Nakama, and Y. Ōnuki, J. Phys. Soc.
Japan 87, 023701 (2018).
[5] K. Kaneko, M. D. Frontzek, M. Matsuda, A. Nakao,
K. Munakata, T. Ohhara, M. Kakihana, Y. Haga, M.
Hedo, T. Nakama, and Y. Ōnuki, J. Phys. Soc. Japan
88, 013702 (2019).

K. Kaneko1,2, M. D. Frontzek3, M. Matsuda3, A. Nakao4, K. Munakata4, T. Ohhara2, M. Kakihana5, Y. Haga6, M. Hedo7, T. Nakama7,
and Y. Ōnuki7
1
Materials Sciences Research Center, JAEA; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center; 3Neutron
Scattering Division, Oak Ridge National Laboratory; 4Neutron Science and Technology Center, CROSS; 5Graduate School of Engineering andScience, University of the Ryukyus; 6Advanced Science Research Center, JAEA; 7Faculty of Science, University of the Ryukyus

32

MLF Annual Report 2018

Research and Development Highlights

In Situ Neutron Diffraction on Phase Transformations fora 1.5Mn-1.5Si-0.2C Steel
1. Introduction
In the past, a steel sample was interruptedly cooled
from an elevated temperature in order to freeze its microstructure and then observations were carried out
at room temperature to monitor the microstructural
evolution during heat treatment. In the case of low alloy steels, austenite phase at a high temperature transforms to martensite during quenching so that the hightemperature microstructure is changed. Therefore, insitu observations of microstructural change during heat
treatment have been attempted by using various techniques like confocal scanning laser microscopy, scanning electron microscopy (SEM)/electron back scatter
diffraction (EBSD), X-ray diffraction and so on. It shouldbe, however, noted that the surface layer of a specimen
is easily damaged at elevated temperatures even in vacuum or inert gas atmosphere; oxidation, decarburization, etc. hinder the collection of real information. In thisstudy, we employed dilatometry, SEM/EBSD observation, X-ray diffraction and in situ neutron diffraction tomonitor phase transformations in situ during heating
and cooling for a Mn-Si-C steel [1, 2].
2. Experimental procedures
The details concerning the specimen preparation
were reported in refs. [1–3]. The chemical compositionsof the steel used were 0.20C-1.50Mn-1.52Si-0.009P0.001S in mass%. The starting microstructure was controlled to consist of ferrite, bainite and austenite. As a
popular experimental method, dilatometry test was
performed, where the specimen was heated with aspeed of 0.05°C/s up to 950°C, held there for 600 s, andthen cooled with 0.05°C/s down to 400°C. In situ SEM/EBSD and X-ray diffraction measurements were carriedout using similar heat history but with step-wise controlof the specimen temperature (the details are covered
in refs. 1 and 2). For in situ neutron diffraction during
heating and cooling, five steel sheets with 1.2 mm inthickness, 30 mm in length and 4–6 mm in width werestacked into nearly cylindrical shape, and set in a conventional dilatometer, which was installed into anengineering neutron diffractometer, BL19, Takumi at
the Materials and Life Science Experimental Facility of
the Japan Proton Accelerator Research Complex (MLF
J-PARC) operated at 400 KW (the maximum designed
power is 1 MW). A slit of 5 5 mm2 for the incident

beam and a 5 mm collimator for the diffraction beam
were used in a medium intensity mode. The specimens
were set in such a way that the angle between the incident beam and the longitudinal direction (rolling direction: RD) of a specimen was 45 degrees. The specimens
were heated to 950°C and cooled with a heating or
cooling speed of 0.05°C/s in vacuum. Using orthogonally installed two detector-banks, diffraction profiles
with respect to RD and ND were recorded simultaneously. The data obtained for every 60 s were analyzed
using the Z-Rietveld code [4].
3. Experimental results and discussion
The obtained dilatometry curve is shown in Fig. 1.
During heating to 950°C and subsequent cooling, thechange in the specimen’s length with temperature wasfound to deviate from the thermal expansion or contraction line, indicating the occurrence of phase transformations. Here, the thermal expansion coefficients offerrite (Kα) and austenite (Kγ) were determined to be 13.5
106/°C and 21.0 106/°C, respectively. This deviation
was attributed to the expansive strain of austenite toferrite transformation. On cooling, the ferrite transformation speed was higher in the beginning, then slowed
down and accelerated again after point P, which is likely
to indicate the onset of pearlite transformation.
Changes in austenite 111 and ferrite 110! peaks
obtained by in situ neutron diffraction during heating
and cooling are shown in Fig. 2 together with the sample temperature as a function of elapsed time. Here,Figure 1. Result of dilatometry test for monitoring phasetransformations [2].

33Research and Development Highlights

MLF Annual Report 2018

Figure 2. Changes in neutron diffraction intensities for 111 austenite (γ) and 110 ferrite(α) with heating and cooling obtained in the axial direction [1].

only the results of cooling [2] are discussed. As seen in
Fig. 2, ferrite transformation started at about 850°C andfinished at 620°C. The austenite volume fraction (fγ) was
determined using the Z-Rietveld software [4]. As seenin Fig. 3, the fγ decreases rapidly in the beginning, thenslows down before the arrowed point P and decreases
rapidly again after the point P with the temperature
reduction. The starting temperature of ferrite transformation shows a good agreement with the result of
dilatometry. Contrary to these neutron results, the transformation temperatures determined either by SEM/EBSD or X-ray diffraction were much higher, because of
the decrease in Mn and C concentrations near the surface at elevated temperatures. Only neutron diffraction
enables us to monitor the bulky averaged information,
which is hardly influenced by surface phenomena.

Figure 3. Change in austenite volume fraction during coolingdetermined by in situ neutron diffraction measurement [2].

34

Different from the dilatometry measurement, in situ
neutron diffraction provides fruitful insights on microstructural change. For example, the lattice parametersof ferrite and austenite were determined using theRietveld analysis and the obtained results are presented in Fig. 4. The austenite lattice parameter is believed
to depend on temperature (T), carbon concentration(C(mass%)) and elastic internal strain (ε), i.e., aγ(T,C,ε).
Similarly, the ferrite lattice parameter is, hereafter, described as aα(T,C,ε) although the carbon content in ferrite is very small. Thermal expansion and contraction
could be satisfactorily fitted by a linear function. For
austenite, the data from 840 to 940°C were expressedby aγ(T,0.20,0)  (0.3580  0.0005)  (7.991  0.006)
106 T (nm) and those from 550 to 610°C for ferrite byaα(T,0,0)  (0.2863  0.0009)  (4.479  0.008) 106 T(nm). Thermal expansion coefficient was calculated using the lattice parameter of 0.3646 nm at 820°C for Kγ
and 0.2889 nm at 575°C for Kα and the obtained resultswere, Kγ  21.9 106/°C and Kα  15.5 106/°C, respectively. These values show good agreement with thosedetermined by dilatometry in Fig. 1.
It is clear in Fig. 4 that the ferrite lattice parameter
deviates from its thermal contraction line. This suggests that compressive internal stress generated due tothe transformation strain in ferrite phase. On the other
hand, the austenite lattice parameter deviates towards
the upper side. This must be due to the internal stresses
balanced with those in ferrite. Another important origin for this deviation would be carbon enrichment. The
deviation from the thermal expansion line is attributed

MLF Annual Report 2018(a) Ferrite

Research and Development Highlights(b) Austenite

Figure 4. Changes in lattice parameters of ferrite (a) and austenite (b) with cooling determined by in situ neutron diffraction
measurement [2].

to transformation strains, thermal misfit strains andcarbon enrichment in austenite. The volume strain of
austenite to ferrite transformation was estimated to be
0.981% [2]. Assuming isotropic expansion, transformatrans  ε trans  ε trans ) are described as ε11tion strains (εtransij
22
33
0.327%. If one computed transformation strains usingtransparameters at 0°C, εv would become 2.3% and then ε11
 0.767%. That is, the strain εv depends on transformais also
tion temperature. As it will be discussed later, εtransij
influenced by the carbon concentration of austenite,which increases with ferrite transformation and lowers. In an austenite-ferrite temperature
the value of εtransij(T)) is generated due
region, thermal misfit strain (εtransij
to the difference in thermal expansion coefficients between austenite and ferrite, which is 6.4 106 (/°C)
estimated from the above results. The thermal history
depends on the time after ferrite forms and could be
calculated as reported in ref. [2]. Several empiricalequations related to the effect of carbon concentration on austenite lattice parameter at RT have been
proposed and the following relationship [5] is adopted
in this study: aγ(RT,C,0)  aγ(RT,0,0)  0.0033C (mass%)
 0.3573  0.0033C (mass%). The estimated aγ(RT,C,0)of 0.35951 nm gave the carbon concentration of
0.667 mass% [2]. The pearlite volume fraction obtained
by SEM microscopy was 26.2%. If the carbon concentration in ferrite and grain boundary segregation were
neglected, the carbon concentration in austenite could
be calculated as 0.20 mass% (bulk average) /0.26 
0.763 mass%. Therefore, pearlite transformation is expected to start when the carbon concentration of austenite is enriched to become approximately 0.7 mass%.
This seems to be reasonable in comparison with thepoint P in Fig. 3. If one estimated the austenite fraction
at P by the so-called lever rule in Fig. 1 using the drawn
thermal contraction lines for ferrite and austenite, itwould be about 10 %, which is much smaller than thosedetermined either by micrography or neutron diffraction. This is because the drawn line is for austenite with
0.2 mass% C not 0.7 mass% C.
The lattice parameter is influenced by the hydrostatic component of elastic strains. During ferrite transformation on continuous cooling, three kinds of eigen
strains (ε*ij) appear as mentioned above. They include
transformation strain (about 0.327%), thermal misfit
strain (about 0.032%) and carbon enrichment in austenite (0–0.647%). The internal stresses are caused by ε*ij,
but high local internal stresses must be relaxed by diffusion and/or dislocation motion at elevated temperatures. The plastic relaxation is too difficult to take into
consideration quantitatively here because its mechanism is uncertain. However, the unrelaxed state could
be evaluated using the Eshelby inclusion theory [2]. Thelong range internal stresses, i.e., phase stresses caused* and σ αby ε*ij can be written as σ γij  fα Cijkl (Sklmn  I)εmnij* (1  fα)Cijkl (Sklmn  I)εmn where Cijkl and I refer to elastic
moduli and unit tensor. Assuming spherical grain and
the Poisson ratio of 0.30, the Eshelby tensor, Sijkl, are ex7  5ν
 0.524, S2233  S3311
pressed as S1111  S2222  S3333  15(1 ν)
5ν  1
 S1122  S3322  S1133  S2211  15(1  ν)  0.0476, S1212  S2323
 5ν)
 0.238. Here, three kinds of origins
 S3131  (415(1  ν)for ε*ij can be regarded to have isotropic feature, ε*ij  qwhen i  j and ε*ij  0 when i " j. Employing the general
γ
γ
γ
 σ22
 σ33
 fα
isotropic Hooke’s equation for Cijkl, σ11(3.57Eq) can be obtained, where E stands for Youngmodulus. Needless to say, the sum of phase stresses iszero and then, ij f  !ij × f!  0. The elastic internalstrain contributing to diffraction peak shift is describedby β11  1 E2ν σ11 where β11  β22  β33  β. Stress or strain
condition is hydrostatic in the present case. Paying attention to austenite phase, tensile hydrostatic strain
increases in the beginning of ferrite transformation
35

Research and Development Highlights

MLF Annual Report 2018

caused by transformation strain and thermal misfit
strain. In conclusion, the lattice parameter of austenite
could be expressed by aγ(T,C,ε)  (aγ(RT,0,0)  0.0033C)(1  KγT)(1  β).
4. Conclusions
The ferrite and pearlite transformation kinetics
showed excellent agreements between dilatometry
and neutron diffraction, whereas the ferrite formation
was observed to start at a much higher temperaturein the X-ray diffraction measurement. Such discrepancy in transformation temperature is attributed to thechange in chemical composition near the surface of a
specimen heated to elevated temperatures; oxidationand changes in Mn and C concentrations were found atnear surface layer after the measurement. In situ neutron diffraction measurement enables us to investigate
the changes in lattice constants of ferrite and austenite,showing not only thermal contraction but also carbon
enrichment in austenite and phase stresses. The transformation strains, thermal misfit strains, carbon enrichment in austenite and generation of phase stresses

during ferrite transformation were discussed from theneutron diffraction data using the Eshelby inclusion
theory. The carbon concentration for the onset of pearlite transformation was estimated and the diffraction
profile line broadening caused by pearlite formation
was presented.
Acknowledgements
This paper is based on the results obtained from a
project commissioned by the New Energy and Industrial
Technology Development Organization (NEDO). The
neutron diffraction measurements were performed at
J-PARC MLF under a user program 2015A0153.
References[1] Y. Tomota, et al., ISIJ Int., 57 (2017), 2237.
[2] Y. Tomota, et al., ISIJ Int., 58 (2018), 2125.
[3] Y. Tomota, et al., Tetsu-to-Hagané, 103 (2017), 573.
[4] R. Oishi, et al., Nucl. Instrum. Meth. A, 600 (2009), 94.
[5] R. C. Ruhl and M. Cohen, Trans. Metall. Soc. AIME,
245 (1969), 241.

Y. Tomota1,2, Y. X. Wang1, T. Ohmura1, N. Sekido1,3, S. Harjo4, T. Kawasaki4, W. Gong5, and A. Taniyama6
Research Center of Structure Materials, National Institute for Materials Science; 2National Institute of Advanced Industrial Science andTechnology; 3Graduate School of Engineering, Tohoku University; 4Neutron Science Section, Materials and Life Science Division, J-PARC
Center, Japan Atomic Energy Agency; 5Elements Strategy Initiative for Structural Materials, Kyoto University; 6Advanced Technology ResearchLaboratories, Nippon Steel Co.

1

36

MLF Annual Report 2018

Research and Development Highlights

Average and Local Structure Analysis of Mn-based Li-ion
Cathode Materials by Neutron and Synchrotron X-ray
Sources
1. Introduction
The lithium ion battery that is currently in use, wasrealized by using LiCoO2 with a layered rock-salt typestructure as a positive electrode material [1]. In recent
years, the attention has focused on the layered type
LiMnO2 [2, 3] or xLi2MnO3-(1x)LiMO2 (M  Mn, Ni, Co)
solid solution [4–8]. However, the layered rock-salt type
LiMnO2 was a metastable phase not synthesized by solid-state method [3, 9, 10]. The crystal structure has notbeen completely revealed [9]. In the average structure
analysis such as Rietveld method, it is difficult to discuss
the effects of substituted Ti distinctly from Mn or solid
solution with disordered arrangements because the Mn
and the substituted elements occupied the same crystallographic site. Therefore, we performed local structure analysis by using a supercell obtained by expanding
the unit cell refined by diffraction study. We focused on
the two Li-ion cathode materials: I. layered rock-salt
LixMn0.9Ti0.1O2 and II. 0.4Li2MnO3-0.6LiMn1/3Ni1/3Co1/3O2.
2. Experimental
The LixMn0.9Ti0.1O2 (x  0.7) was synthesized by
the Na/Li ion-exchange [9, 10]. The 0.4Li 2MnO 30.6LiMn1/3Ni1/3Co1/3O2 was synthesized by co-precipitation method [4–8]. The crystalline phases wereidentified by XRD (X’pert pro, PANalytical) with Cu K!
radiation and by ICP-AES (ICPE-9000, Shimadzu, Ltd.).
The high resolution XRD data were collected by synchrotron XRD at SPring-8 (BL19B2). The diffracted patterns were analyzed by Rietveld method. The X-ray
absorption fine structures (XAFS) were measured at
BL14B2, and their data were analyzed.
Neutron powder diffractions were taken using atime-of-flight diffractometry of iMATERIA (BL20) at the
J-PARC. The structural refinements using neutron diffraction data were performed by Rietveld method using Z-Code [11, 12]. We also performed a high-energy
X-ray diffraction experiment, i.e. total scattering, withan incident beam of 61.5 keV by BL04B2 at SPring-8 andcorrected the obtained data by using a standard program [13]. Neutron total scatterings were collected at
NOVA (BL21), J-PARC. The PDF analysis for total scattering data was performed by PDFgui [14].
The electrochemical cell was constructed using

HS cell (Hohsen Ltd.). The cathode on the Al current
collector consisted of the synthesized active material,
SUPER C65 (IMERYS Co. Ltd.), polytetrafluoroethylene(PTFE). The anode, electrolyte and separator were used
as metal Li, 1 mol/L LiPF6-EC:DMC (1:2 vol. ratio) andpolypropylene (Celgard #2400), respectively. A chargedischarge apparatus (HJ1010m SM8A, Hokuto Denko
Corp.) was employed to conduct the charge/discharge
cycle test at 60°C or 25°C.
3. Results and discussion
3-I. Na/Li ion exchanged LixMn0.9Ti0.1O2
The layered rock-salt structure of LixMn0.9Ti0.1O2 has
not been refined for the broad and unknown peaks in
XRD. We synthesized the material following the method outlined in the previous report. The electrochemical measurements of LixMn0.9Ti0.1O2 were also confirmed
to achieve a relatively high capacity of 215 mAh g1 at
first cycle and 160 mA h1 at 50th cycle. Although the
4 V plateau in the charge and discharge curves indicated the transition to spinel structure, the slightly
changed curves implied the suppression of the spinellization by Ti-substitution [9]. The average structure for
LixMn0.9Ti0.1O2 was analyzed by Rietveld method. The
hexagonal with R–3m space group was adapted to theoriginal structure, where the Mn and Ti, the Li and Na,
and the oxygen were located at 3a, 3b and 6c sites,
respectively. Figures 1(a) and 1(b) show the Rietveld
analysis for LixMn0.9Ti0.1O2 using synchrotron X-ray andneutron diffractions. The results for the LixMn0.9Ti0.1O2
were better fitting, which included no secondary phasebut unknown peaks [9]. The bond valence sum, BVS, of
the oxygen showed almost two by the analysis using
neutron diffraction data, which lead to the better fitting
than synchrotron XRD partly because of the sensitivity
in the neutron for the light elements, Li and O. However,it was inferred that the LixMn0.9Ti0.1O2 was not completely attributed to the layered rock-salt structure and wasconsidered a slightly different structure.
The local structure analysis for the LixMn0.9Ti0.1O2
was performed by the pair distribution function (PDF)
analysis, where the G(r) obtained by the total X-ray andthe neutron total scatterings were used. The two original models were created by the super cell which was37Research and Development Highlights

MLF Annual Report 2018

constructed by the 3a 3b c super cell. One was themodel A defined as the simple expanded cell from theaverage structure analysis. The other was model B, inwhich one of Mn was moved to vacant Li site, assuming
similar coordination of spinel structure. Figures 1(c) and1(d) represented the results for the synchrotron X-ray
and neutron total scattering data of the LixMn0.9Ti0.1O2
using model B, respectively. The refined structures areshown in Fig. 2. The final reliability factors, Rw, were
16.8% and 12.5% for model A and B, respectively. Due
to improved analytical accuracy, it was interpreted that
there must be a local structure similar to the spinel-type.

Once the Rietveld analysis was performed based on thelocal structure model B, the goodness of fit, S2, was improved from 2.437 to 2.425. The Rietveld refinement ofoccupancy for Mn in Li layer lead to the 0.010. Therefore,
the occupation of Mn in the Li layer was supported evenin the diffraction method. Based on the PDF analysis, calculating and averaging the distortion parameters [15],σ2, of TiO6 showed to be smaller than those of MnO6
which were derived from the Jahn-Teller effect in the
Mn3O6 with 3d4 electric coordination. The substitutionof Ti with Mn led to the relaxation in MO6 octahedra andto an improved cycle performance.

(a)

(c)

(b)

(d)

Figure 1. Rietveld analysis for (a) synchrotron XRD and (b) neutron diffraction patterns and PDF analysis for G(r) derived from (c)synchrotron X-ray total scattering and (d) neutron total scattering data in LixMn0.9Ti0.1O2.

(a)

(b)

Figure 2. Refined local structures from super structure of (a) model A or (b) model B in LixMn0.9Ti0.1O2.

38

MLF Annual Report 2018

3-II. 0.4Li2MnO3-0.6LiMn1/3Ni1/3Co1/3O2
At high temperature (HT), the 4.5 V plateau increases derived from the loss of Li2O or O2, yielding a highinitial discharge capacity of 280 mAh/g. As the cycle
proceeded, the polarization became larger and the discharge potential and capacity decreased. We therefore
conducted a local structural analysis using neutron andsynchrotron X-ray total-scattering data to study detailed structural variations associated with the charge/
discharge process. To study PDF data, we created a
3a 2b c supercell (yielding a total of 36 transition-metal atoms) for the initial structural model which followed
a previous study [16]. For the pristine case, we performed a PDF analysis based on the G(r) data obtained
from neutron and synchrotron X-ray total-scattering
measurements. Figures 3(a) and 3(b) show the fitting toneutron total-scattering data, the fitting to synchrotron
X-ray total-scattering data, and 3(c) and 3(d) the structure obtained. The combined analysis yielded a good Rwof 8.69%. The results indicate a layered structure consisting exclusively of TM-O6 octahedra interconnectedin various directions.
Fitting the post-charging models to synchrotron
X-ray total-scattering were performed for the roomtemperature and high-temperature charge at 4.8 V. The
Rw values were 7.64% and 12.33% for the room-temperature (RT) and HT charges, respectively. Because many
Li and O atoms are lost in the HT post-charging, the local structural variations are complicated and thus it ismore difficult to achieve good accuracy in the analysis,so that higher Rw values are obtained compared to the

Research and Development Highlights

pristine. As a result, the structure contained some sites
at which TM-O6 octahedra failed to form due to Li andO loss; nonetheless, no spinel-derived tetrahedral structures were present.
Fitting the post-discharging models to synchrotron
X-ray total-scattering data were also performed for the
RT and HT discharge at 2.5 V. The Rw values were 7.96%
and 8.85%, respectively. The insertion of Li and O atoms
resulted in better fitting accuracy than the post-charging. The structures showed no spinel-derived tetrahedral structures.
In Table 1 we have separately computed distortion parameters for Ni-O6 octahedra in TM layers andin Li layers. The results indicate that the distortion of
Ni-O6 octahedra that mix within the Li layer is particularly reduced at HT compared to RT. This means thatthe capacity is reversible even at HT, which we identify
as one factor responsible for the increase in charging
capacity. At both temperatures, the insertion of Li andO atoms upon discharge causes octahedra to form,
yielding a state close to the pristine. Compared to thepost-charging state, Mn becomes activated after discharge and was reduced from 4 to 3. Because thetrivalent of Mn exhibits a Jahn-Teller distortion, thissuggests that the distortion should increase. However,
we found no evidence for such behavior; instead, thedistortion decreased because of the layered structure
resulting from the formation of octahedra due to Li andO insertion. Meanwhile, the valence of Co and Ni was
reduced during the initial discharge from 4 to 3 andfrom 3 to 2, respectively, and that also contributed

(a)

(c)

(b)

(d)

Figure 3. PDF analysis for (a) neutron and (b) synchrotron X-ray total scattering data in
0.4Li2MnO3-0.6LiMn1/3Ni1/3Co1/3O2 and the local structures (c, d).

39

Research and Development Highlights

MLF Annual Report 2018

Table 1. Distortion parameters of NiO6 octahedra located at TM or Li layer calculated by local
structures from PDF fitting after charge/discharge at RT/HT.

Layer
λσ2 / deg2

Charge (RT)
TM
Li
1.016
1.036
45.72
93.53

Discharge (RT)
TM
Li
1.017
1.019
36.54
40.04

to the reduced distortion. Because TM octahedra tend
to exhibit less distortion at HT than at RT. Similarly tothe post-charging case, the results indicate that the
distortion of Ni-O6 octahedra in both TM and Li layers
was slightly reduced at HT. We attribute the fact that thestructure is preserved at HT despite the loss of many Li,
which yields a large reversible capacity and serves tostabilize the structure.
4. Conclusion
The improvement in cycle characteristics by Ti substitution was due to the existence of a coordination environment similar to the spinel type structure. The Mn
occupied a part of the Li layer and the TiO6 octahedral
distortion was significantly smaller than the MnO6 one.
The influence of Ti substitution on the cathode property of LixMn0.9Ti0.1O2 could be evaluated by the local
structure analysis, which distinguished the partiallysubstituted Ti with the Mn.
Refined distortion parameters of TM-O 6 in
0.4Li2MnO3-0.6LiMn1/3Ni1/3Co1/3O2 revealed their distortions reduced at HT. The Ni-O6 octahedra indicatedthat the mixing introduced less distortion at HT. This
explains why the system retains its structure despite
the loss of many Li at HT and shows the increased discharge capacity. Their details have been published in
papers [17, 18].
References[1] K. Mizushima, P.C. Jones, P.J. Wiseman, J.B.
Goodenough, Mat. Res. Bull., 15, 783–789 (1980).
[2] A.R. Armstrong et al., Nature, 381, 499–500 (1996).

N. Ishida, N. Kitamura, and Y. Idemoto
Faculty of Science and Technology, Tokyo University of Science

40

Charge (HT)
TM
Li
1.017
1.031
34.46
64.19

Discharge (HT)
TM
Li
1.016
1.019
32.67
39.51

[3] A.R. Armstrong, A.J. Paterson, A.D. Robertson, P.G.
Bruce, Chem. Mater., 14, 710–719 (2002).
[4] N. Kumagai, J.-M. Kim, S. Tsuruta, Y. Kadoma, K. Ui,
Electrochim. Acta, 53, 5287–5293 (2008).
[5] N. Tran et al., Chem. Mater., 20, 4815–4825 (2008).
[6] M.M. Thackeray et al., J. Mater. Chem., 15, 2257–
2267 (2005).
[7] T.A. Arunkumar, Y. Wu, A. Manthiram, Chem. Mater.,
19, 3067–3073 (2007).
[8] A. Ito, D. Li, Y. Ohsawa, Y. Sato, J. Power Sources,
183, 344–346 (2008).
[9] N. Ishida, H. Hayakawa, H. Shibuya, J. Imaizumi, J.
Akimoto, Chem. Lett., 41, 1478–1480 (2012).
[10] N. Ishida et al., J. Power. Sources, 244, 505–509(2013).
[11] R. Oishi, T. Kamiyama et al., Nucl. Instrum. Methods
Phys. Res., A600, 94−96 (2009).
[12] R. Oishi, T. Kamiyama et al., J. Appl. Crystallogr., 45,
299−308 (2012).
[13] S. Kohara et al., J. Phys.: Condens. Matter, 19,506101–506115 (2007).
[14] C. Farrow et al., J. Phys. Condens. Matter., 19,335219–335225 (2007).
[15] K. Robinson, G.V. Gibbs, P.H. Ribbe, Science, 172,
567–570 (1971).
[16] Y. Idemoto, Y. Sera, N. Ishida, N. Kitamura,
Electrochem., 83, 879–884 (2015).
[17] N. Ishida, K. Miyazawa, N. Kitamura, J. Akimoto, Y.
Idemoto, Solid State Ionics, 325, 209–213 (2018).
[18] Y. Idemoto, T. Hiranuma, N. Ishida, N. Kitamura, J.
Power Sources, 378, 198–208 (2018).

MLF Annual Report 2018

Research and Development Highlights

Deformation Analysis of Reinforced Concrete Using
Neutron Imaging Technique
1. Introduction
Reinforced concrete (RC), widely utilized for various
architectural and civil engineering structures, is wellknown as a composite structure in which concrete withrelatively low tensile strength and ductility is strengthened by reinforcements such as steel rods (rebars)
with high tensile strength and ductility. The structural
performance of RC is generally derived from the bondresistance between rebar and concrete, which can beassessed by measuring stress distribution along rebar
using neutron diffraction [1]. In addition to that, it isalso important to evaluate the deformation behavior of
concrete around the rebar in order to discuss the mechanism of bond degradation between concrete and rebar. However, it is difficult to see internal deformationof concrete directly even if the neutron diffraction technique is employed, because neutron scattering fromthe hydrogen involved in concrete causes high background noise. Alternatively, image analysis techniques
are typically utilized for evaluating deformation of concrete quantitatively. In this study, therefore, we aim todevelop a novel method to observe internal deformation of concrete using the neutron transmission imaging technique.
2. Experimental procedure
In order to visualize the internal deformation of concrete, cement paste markers containing 34wt% Gd2O3
powder (hereafter called “Gd marker”) were dispersed
as a tracer around rebar in concrete two-dimensionally (Fig. 1). The Gd marker can make strong contrast to
the concrete matrix due to high neutron cross-sectionof Gd. Therefore, the deformation of concrete can bedetected by analyzing the displacement of the Gdmarkers in the neutron transmission image.
The neutron transmission images were taken by
RADEN at BL22 in J-PARC MLF. The L/D ratio of the optical system of RADEN was set to 1000. The incident neutrons scattered and absorbed by the RC specimen weretaken by a cooled CCD camera after being converted tovisible light by a scintillator. The spatial resolution wasapproximately 0.2 mm. The position of the Gd marker ina neutron transmission image of the RC specimen was
evaluated by an image analysis technique described
below using an open source image processing program, ImageJ 1.51n [2].
3. Image Analysis
The flow of the image analysis is shown in Fig. 2.
As shown in a neutron transmission image of the RC
specimen in Fig. 2(a), the Gd markers in concrete canbe recognized clearly. The dark area at the bottom of
the center of the image represents the PVC pipe covering the rebar. In addition, the image contrast between
concrete and the embedded rebar can be observed aswell. The transmission image was normalized by the incident neutron flux and the shade image is depicted inFig. 2(b). And then, the median filter was applied to a
few transmission images taken at the same sample position or at the same loading, in order to remove whitespot noise and to smooth the image. After applying themedian filter, a Fourier transform was applied and thelow frequencies in the transmission image were filteredby masking obtained by a 2D Fourier power spectrum
less than 15 pixels in radius (Fig. 2(c)). After that, thespectrum obtained by excluding the low frequencies

Figure 1. Schematic illustration of the RC specimen used in this study.

41

Research and Development Highlights

MLF Annual Report 2018

Figure 2. Transmission image of the RC specimen (a), and the images for each process, (b), (c), (d)and (e), in the analytical procedure.

was converted to the transmission image using an inverse Fourier transform procedure. This is known asa general high-pass filter, which can highlight the Gdmarker images by reducing the background contrast
variation representing the rebar and the PVC pipe. The
transmission image obtained by the high-pass filter
was binarized by defining an appropriate threshold(Fig. 2(d)). And then, using a morphological process, thespot noise on the obtained binary image was removed
and the Gd marker images were shaped. Eventually, theGd marker images were successfully extracted from theoriginal transmission image as shown in Fig. 2(e). After
extracting the Gd marker images, the center of mass(COM) for each marker was determined by analyzing
particles using ImageJ. In the analysis, particles withless than 300 pixel2 in size (equivalent to the area of acircle with a diameter of 1 mm) were omitted to distinguish from the noise. Furthermore, the particles obviously different from the Gd markers were also regarded
as noise and were manually omitted as well.

42

4. Results and discussion
In order to confirm the spatial resolution of the proposed method, a displacement of the Gd marker image
with respect to the sample stage displacement was verified at first. The displacement of each Gd marker image
was evaluated by a change in the COM of each marker
as a function of the travel distance of the vertical sample stage. As shown in Fig. 3, the average displacement
was linearly plotted with approximately ±0.11 mm
accuracy by image analysis for selected markers withhigher contrast and higher circularity.
Secondary, the deformation of the RC specimen
was measured under compressive deformation by analyzing the displacement of the Gd marker on the transmission image. As shown in Fig. 4, the Gd marker images
move toward the loading direction proportionally tothe applied loading. Furthermore, the displacement of
the Gd marker images are always evaluated to be slightly smaller than the displacement of rebar measured bya displacement transducer, while their trends agree
well within the error bars. This small difference might

Research and Development Highlights

Displacement (mm)

MLF Annual Report 2018

Figure 3. The relation between marker and stage displacements.

Figure 4. The relation between marker displacement andapplied loading, compared with the displacement
measured by a displacement transducer.

be caused by asymmetric distortion of the RC specimen
under pullout loading. Selecting the appropriate Gd
marker with higher contrast and circularity enables us
to analyze deformation inside concrete accurately.

also by increasing statistics accuracy. This method is expected to be utilized for clarifying the bond mechanism
between concrete and rebar by observing concrete
deformation around rebar combined with the bondstress distribution measured by the neutron diffraction
technique.

5. Summary
We have suggested a novel method to observe
internal deformation of concrete by the neutron transmission imaging technique with image analysis. The
measurement accuracy of the Gd marker displacement
can be improved by choosing a spherical shaped Gd
marker, by increasing the contrast of the Gd marker andReferences[1] H. Suzuki, et al., Meas. Sci. Technol., 25 (2014)025602.
[2] C.A. Schneider, W.S. Rasband and K.W. Eliceiri,
Nature methods 9 (2012) 671–675.

H. Suzuki1, T. Koyama2, K. Ueno2, and M. Kanematsu3
Material Sciences Research Center, JAEA; 2Graduate School of Science and Technology, Tokyo University of Science; 3Faculty of Science andTechnology, Tokyo University of Science143Research and Development Highlights

MLF Annual Report 2018

Muon May Reveal the True Worth of “Fool’s Gold”
1. Introduction
Hydrogen is the most ubiquitous element in nature,and occasionally yields an unintended effect on matter.
In today’s electronics industry, hydrogen impurities insemiconductors are known to drastically change theirelectrical activity and characteristic of electronic devices. Hydrogen is the lightest and smallest of all theelements, therefore it is extremely difficult to discern
its states and effect on host materials, especially in low
concentrations. To understand how hydrogen behavesin the semiconductor FeS2, we employed muon-spin rotation (SR) experiments at J-PARC MLF and TRIUMF, aparticle accelerator lab in Canada [1].
2. Pyrite—fool’s gold
Iron disulfide (FeS2), also known as the mineral pyrite
or fool’s gold, has created significant scientific interestand technological applications. It is a promising optoelectronic material due to its suitable indirect band gap
and high absorption coefficient, which opens up great
potential for emerging renewable energy applications,
including photovoltaics, photodetectors, and photoelectrochemical cells [2, 3]. The interest in pyrite has also
been revived due to its low toxicity, virtually infinite elemental abundance, and low raw material cost [4].
The main obstacle to the development of FeS2 as
an optoelectronic material is its low open-circuit photovoltage probably due to unintentional n-type conductivity. Meanwhile, it has been known for decades thatnatural pyrites often exhibit n-type conductivity which
seems to be associated with hydrogen’s defects [5]. So,
one may naturally suspect that hydrogen is the causeof these mysterious electrical activities in FeS2. We cut ablock of natural pyrite into slabs (see Fig. 1) and irradiated them with muon beam to implant muons into FeS2.

(a)

(b)

3. Muogen—pseudo hydrogen
A positive muon () implanted into matter can be
regarded as a light proton isotope in the sense that the
local structure of a muon-electron system is virtuallyequivalent with that of hydrogen. While the light massof a muon (one-ninth that of a proton) often leads tothe isotope effect, which is particularly distinctive in
diffusion at low temperatures, where the quantum tunneling process becomes dominant, a muon also simulates hydrogen diffusion via classical over barrier jumpat high temperatures [6]. Thus, muon in matter can be
regarded as pseudohydrogen. We propose the designation “muogen” (Mu) as the appropriate elemental nameanalogous to hydrogen (see Fig. 2). The electronic stateof Mu can be spectroscopically identified via muonelectron hyperfine parameters using SR techniquewith utmost sensitivity.
4. Local electronic structure of H in pyrite
According to the SR experiment, implanted-muons indicate that there are four electronically inequivalent Mu states in FeS2, i.e., two paramagnetic centerslabeled Mup and Mu#p and two diamagnetic centerslabeled Mud and Mu#d. The magnitude of the hyperfine
parameter [$hf/2  411(40) MHz for Mup and $hf  0 for
Mud], combined with the Hartree potential calculation,suggests that Mup occupies an Fe-tetrahedron center
corresponding to the S-S antibonding site (see Fig. 3).
It is inferred from time-dependent muon polarization that Mup exhibits fast conversion to a diamagnetic state Mu#d ($hf  0, exhibiting depolarization due
to spin/charge exchange interaction), which suggests
the possibility of diffusion-limited trapping of Mup by
defects/impurities to form complex states. Mud is tentatively attributed to an effective-mass-like shallow(c)

Figure 1. (a) Single-crystalline ingot of natural pyrite used in this experiment (unknown origin). (b) Cutting process at the CROSS
user laboratory. (c) Pyrite slabs in the (100) crystal face orientation.

44

MLF Annual Report 2018

Research and Development Highlights

Figure 2. Modified periodic table. Muogen (Mu) is a light pseudo-isotope of hydrogen (H).

Mudinterstitial hydrogen also serves as an electronically active impurity in FeS2.
Comparing predictions from such an analysis withthe results of this experiment could help us uncover thetrue worth of fool’s gold.

Mup

Fe
S
S

Figure 3. Atomic configuration of FeS2 and possible candidate sites for two Mu states (Mup and Mud), where
isosurfaces of the Hartree potential are displayed byblue hatched areas.
donor/acceptor state or a sulfhydryl-like SMu complex
that serves as the donor by releasing an electron upon
formation via the following process: S22  Mu Ѝ S2 
SMu  e.
The small ionization energy (Ep  10 meV for Mup
and Ed  1 meV for Mud) indicates that the electronic levels associated with these Mu centers are situated near(or merged to) the band edge. Meanwhile, the electronic state of Mu#p inferred from a positive frequency shift
under a high transverse field is interpreted as Mup undergoing strong dynamical modulation of $hf, probably
due to fast diffusion. These observations suggest that

Acknowledgements
This work was partially supported by the KEKMSL Inter-University Research Program (Proposal
No. 2016B0011) and by the MEXT Elements Strategy
Initiative to Form Core Research Center for Electron
Materials. We acknowledge CROSS-Tokai for the useof apparatus in their user laboratories and H. Lee for
VASP calculations under the support of KEK Large Scale
Simulation Program No. 16–17.
References[1] H. Okabe, M. Hiraishi, S. Takeshita, A. Koda, K. M.
Kojima and R. Kadono, Phys. Rev. B 98, 075210 (2018).
[2] J. Puthussery, S. Seefeld, N. Berry, M. Gibbs, and M.
Law, J. Am. Chem. Soc. 133, 716 (2011).
[3] D.-Y. Wang, Y.-T. Jiang, C.-C. Lin, S.-S. Li, Y.-T. Wang, C.C. Chen, and C.-W. Chen, Adv. Mater. 24, 3415 (2012).
[4] C. Wadia, A. P. Alivisatos, and D. M. Kammene,
Environ. Sci. Technol. 43, 2072 (2009).
[5] R. Schieck, A. Hartmann, S. Fiechter, R. Könenkamp,and H. Wetzel, J. Mater. Res. 5, 1567 (1990).
[6] H. Graf, G. Balzer, E. Recknagel, A. Weidinger, and R.
I. Grynszpan, Phys. Rev. Lett. 44, 1333 (1980).

H. Okabe1,2, M. Hiraishi1,2, S. Takeshita1,2, A. Koda1,2, K. M. Kojima3, and R. Kadono1,2
Institute of Materials Structure Science, KEK; 2Muon Science Section, Materials and Life Science Division, J-PARC Center; 3Centre for
Molecular and Materials Science, TRIUMF

1

45

Research and Development Highlights

MLF Annual Report 2018

Renormalization of the Spin Excitations in Hexagonal
HoMnO3 by Magnon-Phonon Coupling
1. Introduction
Quasiparticles in condensed matter physics are afundamental concept to understand the excited stateof the system. These particles sometimes interact withthemselves or others. The interactions are usually too
weak to observe, however, the studies about the observation of the strong quasiparticle interaction have beenhighlighted [1–3]. To understand the physics easily, it isrequired to investigate the materials which have a concise structure.
Hexagonal HoMnO3 is a perfect platform to investigate this kind of quasiparticle interactions. The Mn and
Ho planes are well separated and the magnetism is usually dominant by Mn spin. In addition, Mn atoms form
an ideal triangular plane and its magnetic structure is a
non-collinear 120° spin ordered structure. Because thethree-magnon interaction terms are non-zero in noncollinear magnets, we could expect the magnon-magnon interaction. Furthermore, the hexagonal rare-earth
manganite usually has large magneto-elastic coupling
and anomalous features in Raman spectra, ultrasonicwave velocity, inelastic neutron scattering (INS) measurements [4–6]. These indicate that the strong interaction between spin and lattice degrees of freedom ishighly expected in HoMnO3.
In this study [7], we focus on the magnon-magnon
interaction and magnon-phonon interaction in HoMnO3.
We carried out an INS experiment at J-PARC, 4SEASONS
beamline and analyzed the results using three different
calculations, which will be discussed later.
2. Experimental results and discussions
Figure 1 presents the measured spin-wave dispersion along high symmetric momentum points in the 1st
Brillouin zone. Most of the features can be explainedby a conventional 3-sublattice Heisenberg model in atriangular lattice. We considered a nearest-neighbor exchange interaction J and a single-ion anisotropy D andfound that the best fit is J  2.44, D  0.38 meV, which isconsistent with the previous study [8].
However, there are several features that cannot
be captured by the above model. First, the low-energy
magnon dispersion curve located at 11 meV is shifted
downward in comparison with the Heisenberg model. Second, there is a negative slope of the dispersion
along the AB direction, which is not reproduced by any
46

Figure 1. Spin-wave dispersion of HoMnO3. Three different
calculated dispersion curves are plotted together(See the legend) Adapted from the ref. [6].

long-range interactions or exchange anisotropy within
the linear spin-wave theory. Third, the diffusive signals
located at 20 meV are present in the data and they are
not expected in the Heisenberg model.
We tried to explain the anomalies using two different models, which include the magnon-magnon interaction and the magnon-phonon interaction. For themagnon-magnon interaction, we used the XXZ modelwith 1/S expansion [9], which can be described as
HXXZ  J[Six Sjx  Siy Sjy  Siz Sjz ]  O(S1)

(1)

<ij>

To include the magnon-phonon coupling, we also used
an Einstein Site Phonon (ESP) model [10], which is explained by the equation below,
2

HESP = J Si ∙ Sj  cS
→

<ij>

→

2

êOij (Si ∙ Sj)
i 
j%i
→

→

 D (Siz)2 (2)iHere, the constant c indicates the coupling strength between the magnon and phonon.
As already shown in the Fig. 1, both the downward
shift of the magnon energy and the negative slope
along the AB direction are explained by the two models. Using the XXZ model with 1/S expansion, we got
the best fit parameters with J  2.7 meV and Δ  0.88.

MLF Annual Report 2018

For the ESP model, we could obtain the Hamiltonian parameters as J  2.53 and D  0.38 meV. Both parametersexplain reasonably the observations.
Although both the XXZ model with 1/S expansion
and the ESP model describe the same magnon dispersion curves, a critical difference appears in the intensity.
Figure 2 shows the detailed INS data and the intensity
profile of the experimental data and three different calculation models along the AB direction. As shown in
Fig. 2(b), the intensity calculated from the ESP modelis in good agreement with the experimental results.
Especially, the peak ratio located at 11 and 16 meV isonly reproduced by the ESP model. And the diffusive
signals located at around 20 meV is highly expected as
the magneto-elastic excitations, which comes from thehybridization of the magnon and phonon as observedin (Y,Lu)MnO3 [6]. So, we could conclude that the magnon-phonon coupling was the dominant mechanism to
explain the observed anomalies in HoMnO3.
Furthermore, the two-magnon continuum fromthe decay of one-magnon appears to be weak in thedata, which indicate that the magnon-magnon interaction is suppressed in HoMnO3. This is also consistent
with the theoretical estimation. The previous study on
the triangular lattice [9] predicted that if the two-ion
anisotropy 1-Δ in the XXZ model is larger than 0.08, theone-magnon decay is not allowed. Based on our data
and the fit, the 1-Δ in HoMnO3 was found to be 0.12,
which was larger than 0.08. So, we could conclude thatthe magnon-magnon interaction was not the dominantmechanism for the energy renormalization in HoMnO3.
3. Summary
We studied the INS spectra of HoMnO3, which was
the ideal platform to investigate the 2-dimensional
triangular lattice antiferromagnets. We analyzed thedata using three different calculation models, the simple Heisenberg with the single-ion anisotropy, the XXZ
model with 1/S expansion, and the ESP model, to explain all the features. Both the XXZ model and the ESP
model explain the anomalies, but the ESP model explains only the intensity ratio at the B point. Because

Research and Development Highlights

Figure 2. (a) INS data along the AB direction and the three different calculated types of dispersion. (b) The intensity profile at the B point. Adapted from the ref. [6].

of the weak two-magnon continuum and the diffusive
signals at 20 meV expected as the magneto-elastic excitation, we could conclude that the magnon-phonon
coupling was the dominant mechanism for the unconventional spin-wave dispersion in HoMnO3. The magnon-magnon interaction is suppressed in HoMnO3 dueto the large two-ion anisotropy.
References[1] K. W. Plumb, et al., Nat. Phys. 12, 224 (2016).
[2] S. Ito, et al., Nat. Commun. 8, 235 (2017).
[3] T. Kim, et al., J. Phys. Soc. Jpn. 88, 081003 (2019).
[4] A. P. Litvinchuk, et al., J. Phys.: Condens. Matter 16,
809 (2004).
[5] M. Poirier, et al., Phys. Rev. B 83, 054418 (2011).
[6] J. Oh, et al., Phys. Rev. Lett. 111, 257202 (2013).
[7] T. Kim, et al., Phys. Rev. B 97, 201113(R) (2018).
[8] O. P. Vajk, et al., Phys. Rev. Lett. 94, 087601 (2005).
[9] A. L. Chernyshev, et al, Phys. Rev. Lett. 97, 207202(2006).
[10] F. Wang, et al., Phys. Rev. Lett. 100, 077201 (2008).

T. Kim1,2, J. C. Leiner1,2, K. Park1,2, J. Oh1,2, H. Sim1,2, K. Iida3, K. Kamazawa3, and J.-G. Park1,2
Center for Correlated Electron Systems, Institute for Basic Science, Seoul 08826, Korea; 2Department of Physics and Astronomy, Seoul
National University, Seoul 08826, Korea; 3Neutron Science and Technology Center, CROSS
1

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Research and Development Highlights

MLF Annual Report 2018

Structure and Dynamics of Glycine Solution in
Mesoporous Silica
1. Introduction
The separation and purification techniques thatuse mesopores for organic molecules are indispensable
in the field of analytical chemistry, pharmacy and engineering [1]. Although the separation mechanism of
solutes is very complex, its key factors can be attributed
to the interaction between a solute and column walland the confinement effect on an eluent. The interactions between bioorganic molecules and inorganic surfaces have drawn a wide interest due to their significant
role in various fields, including biomineralization [2]and biosensors [3]. With the progress of microanalysis
technology, a technique for immobilizing biomolecules
to solid surface [4] has attracted attention. Therefore, it
is very important to determine the behaviors of soluteand water molecules confined in nano-space.
Glycine, the simplest molecule among amino acids,
is a zwitterion to form NH2/NH3 and COOH/COO
with a pH change of the solution (the isoelectric pointof glycine is 5.47). When observing the change in the
charge state of glycine, the mechanism of interaction
between glycine and silica surface and the hydration
structure of glycine in a confined environment are still
unknown. In the present study, the thermal, structural,and dynamical properties of the glycine solution in micelle-templated mesoporous silica MCM-41 were investigated at pH  5 (neutral) and 2 (acidic) [5].
2. Sample preparation
Mesoporous silica, MCM-41, was synthesized by
Beck’s method. The pore size, the specific surface area,and pore volume of MCM-41 were estimated as 31.3 Å,
723 m2/g, and 0.795 cm3/g by the BJH and BET methods, respectively. The pH of glycine solution is 5 without pH adjustment. By adding hydrochloride solution,
pH of the solution was adjusted to pH  2. A required
amount of the glycine solution and the MCM-41 powder were mixed in an Eppendorf tube. The tube wasvibrated with a vortex mixer for 1 h. The loading ratios(h  mass of glycine solutions/mass of dry MCM-41) ofglycine solution to MCM-41 powder were 0.6 and 0.8.
It was ensured that no exothermic and endothermic
peaks due to freezing and melting of a bulk solution appear in the cooling and heating process of DSC measurements, respectively.

48

3. Thermal and structural properties
Only one peak in the DSC results of confined glycine solution was found, and the melting and freezing
temperatures did not change against the concentrationof glycine. This result indicates that confined glycine solutions at the concentrations measured form eutectic
as well as the bulk. The endo- and exothermic peaks ofconfined glycine solutions were broader than those ofconfined pure water due to the two-phase coexistence
extending down to the eutectic temperature. The melting and freezing temperatures of confined glycine solutions were lower by 10 K than those of confined water.
This finding implies that water structure is disorderedby the hydration of glycine. The enthalpy of fusion ofconfined glycine solution at pH  2 was larger than thatat pH  5, regardless of the glycine concentration and h.
This implies that the charge state of glycine dominantly
affects the water structure in MCM-41.
By subtracting the X-ray diffraction intensity of dry
MCM-41 from that of glycine solution loaded MCM-41,
the radial distribution function (RDF) of glycine solution in MCM-41 was obtained. Compared with RDF
at h  0.8, a shoulder at 2.8 Å in the RDF is seen moreclearly at h  0.6. At the lower loading ratio, the poresof MCM-41 are partially filled with the solution, and theconfined solution would be distributed near the porewall. Compared with the RDFs at pH  2, the small peaks
were observed at 2.65 Å, 3.9 Å, and 5.2 Å in the RDFs at
pH  5. Since the silanol group of MCM-41 is charged
negatively at pH  5, the amino group (NH3) of glycine could interact with the silanol group of MCM-41.
The NMR results of the glycine solution confined inmesoporous silica indicate that the NH3 ՕO-Si bonding could be formed [6]. Therefore, these peaks could
be assigned to N (amino group)  O (silanol group), N(amino group)  Si, and C (carbonyl group)  Si interactions, respectively. This indicates that glycine molecules
are present near the pore wall of MCM-41 at pH  5. On
the other hand, since no such peaks were seen in the
RDFs at pH  2, glycine molecules could be relatively
hydrated by confined water. Thus, the liquid structureof the glycine solution in MCM-41 at pH  5 and 2 is illustrated in Fig. 1. To verify the surmise, the dynamics ofglycine and water is investigated.

MLF Annual Report 2018(a) pH  5

Research and Development Highlights(b) pH  2

Figure 1. Illustrations of the liquid structure of glycine solution in MCM-41 at (a) pH = 5 and (b) 2.

1
S(Q,ω)  C(Q)∙δ(ω)  D(Q) 
R(Q,ω)  BG ,

Γ(Q)(ω2  Γ(Q)2)(1)
where C(Q) and D(Q) are intensities of elastic and QENS
components, respectively. Γ(Q) is the half-width at halfmaximum of Lorentzian function, reflecting the translational diffusion of water and glycine molecules. BG isthe background, and R(Q,ω) is the resolution function.
Since the incoherent scattering cross-section of
protons is larger by a factor of 40 than those of theother atoms, the dynamics of glycine molecule would
be obtained from the result of H-Gly/D2O solution,

whereas the dynamics of water molecule would be derived from the result of the D-Gly/H2O solution.
Figure 2 shows the Q dependence of Γ(Q) of confined H-Gly/D2O at pH  5. Since the translational motion is faster at a higher temperature, the Lorentziancomponent in the spectrum becomes wider. Hence,
the fitting of the model became difficult under theincreasing temperature. Moreover, the QENS spectra
at Q2 & 2 Å2 were not analyzed since the elastic peak
due to the scattering of MCM-41 was not negligible
in the Q-range. The activation energy of the diffusion
constant was calculated from the Arrhenius plot of diffusion constants (Fig. 3). The activation energies of thewater molecule at pH  5 and 2 are 20.9  1.2 and 21.8
 1.5 kJ/mol, respectively. The activation energy of thetranslational motion of water in confined glycine solutions is comparable to that of pure water confined in
MCM-41 (21.6 kJ/mol) [7] but is larger than that of bulk

H-Gly solution at pH=5 in MCM-41
20

305 K
290 K
275 K

HWHM / μeV

4. Dynamics of glycine and water in MCM-41
Two kinds of glycine solutions (deuterated glycine/
H2O and glycine/D2O) were prepared; these are abbreviated to D-Gly/H2O and H-Gly/D2O. The powder samples
were wrapped with a sheet of aluminum foil (20 m
thick). Then, it was bent cylindrically and inserted intoa cylindrical aluminum cell of 14.0 mm in inner diameter, 0.25 mm in thickness, and 50 mm in height. The
QENS measurements were carried out using a time-ofﬂight near backscattering spectrometer DNA (BL02),
and the energy transfer of neutrons by scattering, $,varied within 20100 eV. The QENS measurementsof the samples were performed at 245–305 K. The sample was measured at 100 K to estimate the instrumental
resolution.
QENS spectra, S(Q,ω), reflect translational and rotational motions. In the present experiment, since thespectra which arise from the rotational motion are muchwider, compared with the observable energy range ofthe spectrometer, the contribution from the molecularrotation is included in a background term. Therefore,
S(Q,ω) was analyzed by a model of translational diffusions of water and glycine molecules as follows:

260 K

10
245 K

0

0

1
2

Q /Å

2
−2

Figure 2. Q dependence of the width of a Lorentzian function of H-Gly/D2O at pH = 5 in MCM-41. The solidline shows the results according to the jump diffusion model.

49

Research and Development Highlights

MLF Annual Report 2018

D/m s

2 −1

D-Gly pH=5
D-Gly pH=2
H-Gly pH=5
H-Gly pH=2
−9

10

−10

10

3

3.5
−1

4
3

T ×10 / K

−1

Figure 3. Arrhenius plot of diffusion constants of glycine andwater molecules in confined solutions at pH = 5
and 2.

water (17.9  0.9 kJ/mol) [8]. This would be due to theattractive interaction between water and silanol groupof the MCM-41 wall. On the other hand, the activationenergies of the translational motion of glycine at pH  5
and 2 are 19.3  1.1 and 17.0  0.8 kJ/mol, respectively.
The activation energy of translational motion of glycine
at pH  5 is larger than that at pH  2. These results canbe explained by the attractive interaction of glycine
molecules with the silica wall of MCM-41, as seen in the
RDF of glycine solution in MCM-41 at pH  5.
NMR results of a glycine solution confined inmesoporous silica indicate that the NH3 ՕO-Si bonding could be formed [6]. However, some DFT calculations of the system of glycine, water, and silica revealed
that the direct hydrogen bonds of CO ՕHO-Si areformed, and that NH3 interacts with O-Si via a watermolecule [9]. The RDFs in the present study could not
rule out the possibility of forming the direct hydrogenbonds of CO ՕHO-Si.
Further work, such as neutrons diffraction with
14N/15N isotope substitution is needed to clarify this issue. The silanol group of MCM-41 is charged positively
at pH  2 [10], and a glycine molecule also has a positive charge at pH  2 which is lower than the isoelectric point. Under this situation, the repulsive interaction
between the glycine molecule and silanol group would
keep glycine molecules away from the wall of MCM-41.

Consequently, water molecules will be adsorbed on thewall of MCM-41 instead of glycine molecules. The present results are expected to give essential knowledge
about the interaction between bioorganic molecules
and inorganic surfaces and to improve technique forimmobilizing biomolecules to microchannels.
5. Future perspectives
The present result demonstrated that quasi-elastic
neutron scattering with H/D substitution could clarify
the dynamical behavior of solute and water in confinednano-space. For further applications, the analysis ofdynamical behavior in mesoporous silica nanoparticle(MSN) will continue. Since MSN has the size of few tensof nm and biocompatibility, MSN can penetrate theliving cell [11]. The application of the loading of small
molecules as well as macromolecules such as proteins,siRNA is being developed. Thus, MSN is attracting attention as a material for elucidating cell dynamics. Neutron
beams can become strong tools to uncover life phenomena from the perspective of physical science.
References[1] S. Ahuja et al., Handbook of Pharmaceutical
Analysis by HPLC (Academic Press, 2005).
[2] S. Mann, Biomineralization: Principles andConcepts in Bioinorganic Materials Chemistry(Oxford University, New York, 2001).
[3] K.Besteman et al., Nano Lett. 3, 727–730 (2003).
[4] K. Nakanishi et al., J. Biosci. Bioeng. 91, 233–244(2001).
[5] K. Yoshida et al., J. Chem. Phys. 149, 124502 (2018).
[6] I. B. Shir et al., J. Phys. Chem. C 116, 9691–9702(2012)[7] T. Yamada et al., J. Phys. Chem. B 115, 13563–13569(2011).
[8] S. Takahara et al., J. Phys. Chem. B 103, 5814–5819(1999).
[9] A. Costa et al., Phys. Chem. Chem. Phys. 10, 6360–
6368 (2008).
[10] G. E. Musso, et al., Phys. Chem. Chem. Phys., 17,13882-94 (2015).
[11] R. Narayan et al., Pharmaceutics 10(3), 118 (2018).

K. Yoshida1, T. Inoue1, M. Torigoe1, T. Yamada2, K. Shibata3, and T. Yamaguchi1
Fukuoka University; 2Neutron Science and Technology Center, CROSS; 3Neutron Science Section, Materials and Life Science Division,
J-PARC Center

1

50

MLF Annual Report 2018

Research and Development Highlights

Topological Transitions among Skyrmion- andHedgehog-Lattice States in Cubic Chiral Magnets
1. Introduction
Topological spin textures such as skyrmions andspin hedgehogs (Fig. 1) give rise to novel emergent
properties, which can be exploited for spintronic functionalities [1]. Whereas the formation or deletion process of them has been intensively studied, switchingof spin textures among different topological orders remain largely unexplored.
We have investigated the topological transitions
among skyrmion lattice (SkL) and hedgehog lattice (HL)in new chiral magnets MnSi1xGex. By changing chemical pressure through substitution between Si and Ge,
we have discovered that the SkL in MnSi undergoes
two-step transitions to the cubic-3q HL in MnGe (Fig. 2).
In the intermediate composition range (x  0.3 – 0.6),
we have unveiled a new topological spin texture characterized four wavevectors (q-vectors), i.e., tetrahedral4q state (Fig. 1(b)).

(a)

(b)

(c)

Figure 1. Schematics of topological multiple-q spin textures.
The tetrahedral-4q HL is a new topological spin texture which has been identified in our work.

Figure 2. Variation of magnetic phase diagram in MnSi1−xGex.
The drawn phase boundary line for each x represent the ferromagnetic transition.

2. Experiment
Neutron scattering experiments were performed atsmall- and wide-angle neutron scattering instrument(TAIKAN) built at BL15 of MLF. A powder sample of polycrystalline MnSi1xGex, synthesized by high-pressuretechnique, was packed in an aluminum container filled
by He gas and installed in a cryomagnet. Magnetic field
was applied perpendicular to the incident neutron
beam. The diffracted neutron beam with the wavelength of 0.5  λ  7.8 Å was collected by four detectorbanks of small-, middle-, and high-angle and backward
detector banks, and analysed by using time-of-flight(TOF) method.
3. Result
In order to clarify the variation of magnetic period(λ) and direction of q-vectors in MnSi1xGex, small- andwide-angle neutron scattering experiments were performed at zero magnetic field. Figure 3(a), (b) show thesmall-angle neutron scattering (SANS) intensity patternsof x  0.6 and 0.8 after zero field cooling from room temperature. The observed Debye-ring-like patterns indicate the formation of periodically modulated magnetic
structures. Their modulation periods are determinedfrom the radius (q) of the diffracted ring pattern as λ 
2π/q, which we will be discussed in the later section.
The q-vectors, which are fixed along specific crystal-axes due to magnetic anisotropy, were identified bywide-angle neutron scattering. Figure 3(c), (d) show the51

Research and Development Highlights

(a)

(c)

MLF Annual Report 2018

(b)

(a)

(d)
(b)

Figure 3. The SANS intensity patterns ((a), (b)) and powder
neutron diffraction patterns around (100) nuclear
reflection ((c), (d)) after zero-field cooling.

wide-angle neutron diffraction profiles around (110)
nuclear reflection. Because magnetic reflections generally appear as satellite peaks at the wavenumber of|qnq| in a powder neutron diffraction, we can determine the q-direction from the satellite peak position
once we identify the magnitude of q by SANS. Here, qn
is the reciprocal lattice vector. Each satellite peak observed in x  0.6 and 0.8 (indicated by blue and red tri—
angles in Fig. 3(c), (d)) can be indexed as (2π ⁄a  q ⁄√ 3,——
2π ⁄a  q ⁄√ 3, q ⁄√3 ) and (2π⁄a  q , 2π⁄a, 0), respectively (ais lattice constant). Namely, the q-vector directions arealong 111& crystal axes for x  0.6, and 100& crystal
axes for x  0.8.
Next, we investigated the magnetic structures under magnetic field by SANS in x  0.2, 0.6, 0.8. Magnetic
field (H) is applied perpendicular to the incident neutron beam. As shown in Fig. 4(a), the SANS pattern ofx  0.2 exhibits intensity peaks parallel (φ  0°, 180°)
and perpendicular (φ  90°) to H, which indicates theconical state modulating along H coexists with SkL. We
also confirmed that the peaks at φ  90° only emerge
in the SkL phase identified by the magnetization
measurements.
In x  0.6 and 0.8, we also detect characteristic SANS
patterns under H: In addition to the intensity peaks at φ
 0°, 180°, there appears peaks at φ  70°, 110° for x 
0.6 and at φ  90° for x  0.8. We interpret these SANS
patterns in terms of multiple-q structures. As for x  0.6,
Fig. 4(b) illustrates the possible multiple-q structure explaining the SANS result, i.e., the tetrahedral-4q state.
As for x  0.8, the observed intensity pattern is identical to that of MnGe where the cubic-3q HL is realized(Fig. 4(c)) [2, 3].
52(c)Figure 4. The SANS intensity patterns under magnetic field
and the candidate multiple-q states explaining theresults.

We note that we cannot exclude a possibility ofmulti-domain state of the single-q helical structure on
the basis of the SANS results alone. However, such a
scenario is incompatible with the observation of large
topological Hall effect (THE), which is the hallmark of
the formation of non-coplanar spin textures endowedwith scalar spin chirality (data not shown). Indeed, we
observed THE with distinct features unique to each topological phase realized in MnSi1xGex.
4. Discussion
We have unveiled the transitions among distinct
topological spin textures, namely SkL and two classes
of HLs in cubic chiral magnets MnSi1xGex. It is noteworthy that the observed topological transitions canbe driven essentially by the lattice constant change.
One important indication we obtain is that the dominant magnetic interactions for HL may differ from thosefor SkL where the competition between ferromagnetic
exchange interaction (EXI) (JSi ∙ Sj) and DzyaloshinskiiMoriya interaction (DMI) (D ∙(Si Sj)) determines themagnetic period as λ  a∙J ⁄D. In the conventional SkL
materials, the magnetic ground state is a long-period
helical structure (λ  10–100 nm) since the energy scale

MLF Annual Report 2018

Research and Development Highlights

is well-separated as J » D. If the same model could beapplied, the extremely short λ (1.94–2.80 nm) observedin MnSi1xGex (x  0.4–1) (Fig. 5) would require muchlarger DMI even exceeding EXI, which is not consistent
with our first-principles calculation.
Thus, DMI may not be the primary origin of theshort-period helical structure in HL. Instead, the magnetic frustration or Ruderman-Kittel-Kasuya-Yoshida(RKKY) interaction causing competing ferromagnetic and anti-ferromagnetic EXIs can be a possible
mechanism.

Figure 5. Variation of magnetic period (λ) in MnSi1−xGex. The
extremely short in x = 0.4–1 is beyond the understanding of conventional paradigm based on Dzyaloshinskii-Moriya interaction.

References[1] N. Nagaosa and Y. Tokura, Nat. Nanotech. 8, 899(2013).
[2] N. Kanazawa et al., Phys. Rev. Lett. 106, 156603(2011).
[3] N. Kanazawa et al., Phys. Rev. B 86, 134425 (2012).

Y. Fujishiro1, N. Kanazawa1, T. Nakajima2, X. Z. Yu2, K. Oishi3, Y. Kawamura3, K. Kakurai2,3, T. Arima2,4, H. Mitamura5, A. Miyake5,
K. Akiba5, M. Tokunaga5, A. Matsuo5, K. Kindo5, T. Koretsune6, R. Arita1,2, and Y. Tokura1,2
1
Department of Applied Physics, The University of Tokyo; 2RIKEN, CEMS; 3Neutron Science and Technology Center, CROSS; 4Department ofAdvanced Materials Science, The University of Tokyo; 5ISSP, The University of Tokyo; 6Department of Physics, Tohoku University

53

Research and Development Highlights

MLF Annual Report 2018

2D Bragg-Edge Elastic Strain Tomography
Background
The rapid development of pixelated time-of-flightneutron detectors has given prominence to Bragg-edgetransmission geometry as an excellent approach forelastic strain measurement in polycrystalline materials(see Fig. 1(a)). Bragg-edges refer to abrupt increases
in the transmission rate in polycrystalline samples atwavelengths corresponding to back scattered neutrons.
Relative shifts in the location of these edges can provide
a measure of elastic strain in much the same way as
traditional diffraction techniques. Along with the development of pixelated time-of-flight detectors, significant
interest in strain imaging techniques and the associated‘rich’ tomography problem has been generated. The
state-of-the-art due to Tremsin is now capable of twodimensional strain imaging with spatial resolution down
to 55 m (e.g. [1]).
Several attempts have been made at solving the associated tomographic reconstruction problem over the
past decade. As opposed to conventional tomographic
imaging, this problem focuses on the reconstructionof a tensor field, which is a significantly more complex
problem.
Bragg-edge strain tomography has the potential
to transform the way in which experimental mechanics
is carried out. In much the same way that regular CT
transformed medicine and other sciences, a full-fieldapproach to measuring strain distributions within engineering materials may have an impact across a rangeof areas. One obvious example is in the developmentof novel manufacturing processes such as 3D printing.
Residual stress locked in by the printing process has acritical impact on the strength of the resulting parts; thismust be understood in order to advance the technology.
In contrast to X-ray and pointwise neutron diffraction
techniques, Bragg-edge strain tomography promises toreveal the full three-dimensional distribution of strain
throughout printed engineering parts over the scale ofcentimeters.
A recent paper by Lionheart and Withers [2], andprior work by Sharafutdinov [3], clearly demonstrated
that the problem was mathematically ill-posed. The issue revolves around the fact that multiple strain fields
can project to the same set of strain images; solutions to
the tomography problem are not unique. This does notprohibit reconstruction in general, however it does meanthat additional information is required. Historically, this information has taken the form of assumptions (i.e. special
cases). As an example, much of the initial work in this area
was limited to assumptions of axial symmetry (e.g. [4]).
A reconstruction algorithm for the special case of strain
fields resulting strictly from in situ applied loads has also
been developed and demonstrated experimentally [6, 7].
Recent work by the authors has provided a path togeneral reconstruction through consideration of known
physical constraints, such as equilibrium. Through thisapproach, we have been able to demonstrate tomographic reconstruction of two-dimensional residualstrain fields (plane-stress) in simulation, and, as outlinedin this paper, from experimental measurements.

(a)
(b)

Figure 1 (a) Bragg-edge imaging on a pulsed neutron source. (b) Transmission geometry and coordinate system.

54

MLF Annual Report 2018

Reconstruction
Mathematically, Bragg-edge strain measurement is
described by a generalization of the well-known Radontransform known as the Longitudinal Ray Transform(LRT);
1 Lϵ (x  sn̂ )n̂ n̂ ds
ϵ (p,θ) i j
L ∫0 ij 0
where, with reference to Fig. 1(b), ϵ is the strain fieldwithin the sample, n̂  [cos θ sin θ ]T is a unit vector in
the direction of the beam, xo is the point of entry into
the sample, and s is measured along the path of length
L through the sample.
As discussed earlier, the LRT has a non-trivial nullspace which prohibits its direct inversion. Additional
information is required, and, in our work, this takes theform of an assumption of mechanical equilibrium. Thisis implemented through the concept of stress functions
from which the unknown stress is defined in a way that
automatically satisfies the well-known equations ofequilibrium. In 2D (i.e. plane stress or plane strain), Airy
stress functions provide a good example whereby the
unknown components of stress can be defined as;

(a)

(b)

Research and Development Highlights

σij 

∂2 φ
∂ i ∂jfor an arbitrary (unknown) Airy stress function φ.
Together with Hooke’s law to relate stress andstrain, we can tomographically reconstruct φ fromthe observed strain images in order to establish the
unknown strain field. Practically, this can be achieved
through a number of techniques; our approach has involved the implementation of Gaussian Process (GP) regression. Through the GP approach we have also beenable to include other known constraints such as, in thecase of residual stress samples, the absence of externally applied loads. A full description can be found in [11].
Experimental Demonstration
An experimental demonstration of this technique
has been carried out using a set of strain images measured on the RADEN (Energy Resolved Neutron Imaging)
instrument at J-PARC. This experiment focused on
two samples (see Fig. 2(a)); 1. A crushed steel ring, and
2. An offset steel ring-and-plug. All details of the sample
design, experiment set-up, and strain measurement can befound in [9]. For context, we provide the following summary.

(c)

(e)

(f)

(d)

Figure 2 (a) Sample geometry; upper - crushed ring, lower - asymmetric ring-and-plug. (b) and (c) Transmission strain profiles
were measured from the two samples simultaneously on RADEN. (d) The resulting strain-sinograms; left - crushed ring,right - asymmetric ring-and-plug. (e) and (f ) Reconstructions compared to constant wavelength strain scans from KOWARI(measurement locations indicated by data points).

55

Research and Development Highlights

MLF Annual Report 2018

The two samples were constructed from the samebar of EN26 low-carbon/high alloy steel. The first sample was plastically defomed by 1.5 mm on the diameterto create a residual strain field, the second contained
a residual stress field resulting from interference between the ring and a plug using a shrink-fit assembly
process. Both samples were 14 mm thick, allowing
them to be stacked within the field of view of a 10B MCP
pixelated ToF detector [1] (see Figs. 2(b) and 2(c)). A setof 50 strain images was measured over golden angle
increments of rotation. Measurements were performed
over columns of pixels spanning the thickness of thesample to provide one-dimensional projections of thetwo-dimensional strain field. In total, 20,664 individual
measurements were collected over the 50 projections,each with a measurement uncertainty around 104.
The resulting strain-sinograms are shown in
Fig. 2(d), from which we were able to reconstruct thestrain fields shown in Figs. 2(e) and 2(f ). These reconstructions are shown in comparison to detailed strainscans carried out on the KOWARI strain diffractometerat the Australian Centre for Neutron Scattering within
ANSTO (0.5 0.5 14 mm gauge volume). Two separate
reconstructions are shown; 1. A reconstruction constrained only by equilibrium, and 2. A reconstruction
constrained by both equilibrium and an absence of surface traction. Both reconstructions agree well with thetraditional strain scan, however the second one showsmuch greater fidelity.
Conclusions
Bragg-edge elastic strain tomography for general
strain fields has been successfully demonstrated using
the RADEN energy resolved imaging instrument within
J-PARC. The approach we have developed has a naturalextension to three dimensions (i.e. triaxial strain fields)
and our current work is focused on achieving this goal.

References[1] AS Tremsin et al. “High-resolution strain mapping
through time-of-flight neutron transmission diffraction with a microchannel plate neutron counting detector”, Strain, 48:296–305, 2012.
[2] WRB Lionheart and PJ Withers. “Diffraction tomography of strain”, Inverse Problems, 31:045005, 2015.
[3] VA Sharafutdinov. “Integral geometry of tensor
fields” VSP, The Netherlands, 1994.
[4] HJ Kirkwood et al. “Neutron strain tomographyusing the radon transform”, Mat. Today: Proc.,
2:S414-S423, 2015.
[5] CM Wensrich et al. “Neutron transmission strain
tomography in granular systems” Strain, 52:80–87
2016.
[6] CM Wensrich et al. “Bragg-edge neutron transmission strain tomography for in situ loadings”, Nucl.
Inst. & Meth. in Phys. Res. B, 383:52–58, 2016.
[7] JN Hendriks et al. “Bragg-edge elastic strain tomography for in situ systems from energy-resolved neutron transmission imaging”, Phys. Rev.
Mat. 1:053802, 2017.
[8] AWT Gregg et al. “Tomographic reconstructionof residual strain in axisymmetric systems from
Bragg-edge neutron imaging”, Mech. Res. Comm.
85:96–103, 2017.
[9] AWT Gregg et al. “Tomographic reconstruction of
two-dimensional residual strain fields from Braggedge neutron imaging”, Phys. Rev. App. 10:064034,
2018.
[10] C Jidling et al. “Probabilistic modelling and reconstruction of strain”, Nucl. Inst. & Meth. in Phys. Res. B.
436:141–155, 2018.
[11] JN Hendriks et al. “Implementation of traction constraints in Bragg-edge neutron transmission strain
tomography”, Strain (arXiv:1805.09760v2), 2018 (inPress).

C. M. Wensrich1, A. W. T. Gregg1, J. N. Hendriks1, A. S. Tremsin2, T. Shinohara3, V. Luzin1,4, A. Wills1, O. Kirstein1,5, M. H. Meylan6,
and E. H. Kisi1
1
School of Engineering, The University of Newcastle; 2Space Sciences Laboratory, University of California; 3Neutron Science Section,
Materials and Life Science Division, J-PARC Center; 4Australian Centre for Neutron Scattering, ANSTO; 5European Spallation Source;
6School of Mathematical and Physical Sciences, The University of Newcastle

56

MLF Annual Report 2018

Research and Development Highlights

Crystalline Electric Field Level Scheme of the NonCentrosymmetric CePtSi3
Introduction
The study of new phenomena that appear due to alack of inversion symmetry, such as spin Hall effect, multiferroics, topological insulators, and parity-mixing superconductors, has become one of the trends in modern
physics. Especially, interesting phenomena such as unconventional pressure-induced superconductivity andmultiple metamagnetic transitions have been reported
in the CeTSi3 system with a non-centrosymmetry (T transition metals) [1, 2]. As a starting point of researchon the CeTSi3 system, we chose CePdSi3 which has notbeen reported as superconductive by polycrystalline
studies. We grew a single crystalline sample and measured the specific heat and magnetization to estimate
the crystalline electric field (CEF) level scheme [2]. These
results were in good agreement with the results of inelastic neutron scattering (INS) experiments reported
in previous researches [3] and revealed that the wave
function of the ground state of CePdSi3 was 6. Knowing
the CEF levels in the CeTSi3 systems, we noticed that theprevious study on CePtSi3 claimed that the CEF level lies
at anomalously high energy [4]. Therefore, in the present study, we examined the CEF excitations in CePtSi3
by INS experiment with a polycrystalline sample.

polycrystalline sample. The obtained sample was enhanced by annealing at 1050°C for 1 week.
INS experiments were carried out on polycrystalline samples of CePtSi3 and LaPtSi3 using the High
Resolution Chopper (HRC) spectrometer installed at
BL12 in J-PARC MLF. Nonmagnetic and isostructural
LaPtSi3 was used to estimate the phonon contribution
to the scattering. Samples were cooled to 2.8 K, and INS
spectra were acquired with three incident energies Ei 
11, 50, and 258 meV.
Results and discussion
Color-coded |Q|-E plots of the INS intensities of
CePtSi3 are shown in Figs. 1(a) and 1(b) [5]. Figure 1(a)shows the data at Ei  258 meV, and no excitation was observed around 86 meV at which the previous magnetic
susceptibility analysis suggested one of the CEF excitations [4]. By contrast, CePtSi3 clearly shows the magnetic
scattering below 20 meV as seen in Fig. 1(b) which was
obtained by Ei  50 meV. Here, we subtracted the phonon contribution of CePtSi3 which was evaluated fromthe observed phonon spectrum in LaPtSi3. The CEF excitations have been observed at approximately 5.3 and17.5 meV, as indicated by the black arrows in Figs. 1(b)and 1(c). To see the CEF excitation peaks more clearly,
the 1D-cut of Fig. 1(b) was constructed by integrating
the intensity at |Q|  3 Å1 over the width of 0.1 Å1 andshown in Fig. 1(c). The inset shows the expanded profile
observed with Ei  11 meV to better resolve the lower

Experimental procedure
The constituent elements (Ce, 3N; La, 3N; Pt, 3N;
Si, 6N) of Ce: Pt: Si  1: 1: 3 were melted on a watercooled copper hearth in an arc furnace to obtain a(b)
CePtSi3
T = 2.8 K
Ei = 258 meVE [meV]

30

100

−8

1.0×10CePtSi3
T = 2.8 K
Ei = 258 meV

0.8
6×10
5
4

20

3
2
1

10

50

0

2

4

6

8
−1

|Q| [Å ]

10

12

0
0

1

−9

3.0×105.3 meV

2.5

2

3
−1

|Q| [Å ]4

5−9

Intensity [arb. unit]

E [meV]

150

0
0

(c)
40

Intensity[arb. unit]

200

Intensity [arb. unit]

(a)

0.6

2.0
1.5
1.0

CePtSi3
Ei = 11 meVconst. |Q|[1.2 – 1.4]

0.5
0
−2

0.4

0

17.5 meV468E [meV]

CePtSi3
const. |Q|[2.9 – 3.1]

0.2
0
−10

2

0

10

20

30

40

50

E [meV]

Figure 1. Color-coded plots of the INS intensity (a) with Ei = 258 meV and (b) magnetic scattering with Ei = 50 meV of CePtSi3 at 2.8 K.
(c) is a cut of magnetic scattering integrated over |Q| from 2.9 to 3.1 Å−1, and the inset shows the cut integrated from 1.2
to 1.4 Å−1 measured with Ei = 11 meV. The black arrows indicate the positions of the two CEF excitations at approximately
5.3 and 17.5 meV [5].

57Research and Development Highlights

MLF Annual Report 2018

peak at 5.3 meV. The result of the CEF model calculation,
which takes into account the observed CEF excitations,explains well the behavior of the specific heat and themagnetization, and we established that the wave function of the ground state of CePtSi3 is 6. The level scheme
of CePtSi3 is in qualitatively good agreement with theresult of CePdSi3 [2, 3]. We note that although the wave
function of the ground state of pressure-induced superconductors CeRhSi3 and CeIrSi3 is 7, the ground stateof CePdSi3 and CePtSi3 with the multiple metamagnetictransitions is 6. In the CeTSi3 system, the differences in
the physical properties such as superconductivity andmultiple metamagnetic transitions may be classified by
the wave function of the ground state.

References[1] N. Kimura, K. Ito, H. Aoki, S. Uji, and T. Terashima,
Phys. Rev. Lett. 95, 247004 (2005) etc.
[2] D. Ueta, Y. Ikeda, and H. Yoshizawa, J. Phys. Soc. Jpn.
85, 1014703 (2016).
[3] M. Smidman, Ph.D. thesis, The University of Warwick(2014).
[4] T. Kawai, Y. Okuda, H. Shishido, A. Thamizhavel, T.
D. Matsuda, Y. Haga, M. Nakashima, T. Takeuchi, M.
Hedo, Y. Uwatoko, R. Settai, Y. Ōnuki, J. Phys. Soc.
Jpn. 76, 014710 (2007).
[5] D. Ueta, T. Kobuke, M. Yoshida, H. Yoshizawa, Y.
Ikeda, S. Itoh, T. Yokoo, Physica B 536, 21 (2018).

D. Ueta1,2, T. Kobuke1, M. Yoshida1, H. Yoshizawa1, Y. Ikeda3, S. Itoh4,5, and T. Yokoo4,5Institute for Solid State Physics, University of Tokyo; 2Okinawa Institute of Science and Technology Graduate University; 3Institute forMaterials Research, Tohoku University; 4Neutron Science Section, Materials and Life Science Division, J-PARC Center; 5Institute of Materials
Structure Science, KEK

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MLF Annual Report 2018

Research and Development Highlights

Observation of Temperature-Induced Structural
Transition of Ceria via Solid-Gas Reaction
1. Introduction
Monitoring solid-gas chemical reactions is important not only in general chemistry but also in industrial
applications. In the three-way catalysis (TWC) used in
the automotive industry, the catalysts undergo a crystal structure change at high temperatures in a gas
atmosphere.
Cerium dioxide (ceria or CeO2) plays an extremely
important role in TWC. This is attributed to the high oxygen storage capacity of CeO2 resulting from the spontaneous redox reaction of cerium (CeIV ' CeIII) [1]. Underhydrogen atmosphere, CeO2 forms complex oxygendeficient structures with a stoichiometric composition
or non-stoichiometric compositions [2–4]. On the other
hand, the diverse structure, which is the hydrogencontaining ceria (HyCeO2), was predicted by a calculation [5]. Although experimental and simulation studies
showed that hydroxyls are formed by hydrogen [6–8],
the chemical reaction and the crystal structure have notbeen experimentally observed yet.
In general, the reduction is explained by the reaction kinetics, which depends on temperature. To elucidate the structural changes in ceria under hydrogen,the investigation of the isothermal holding time andthe crystal structure after thermal treatment is important. Herein, we investigated the crystal structure of ceria depending on the isothermal holding time at hightemperature and various temperatures under hydrogen by using in situ neutron powder diffraction (NPD).
2. Experimental
We performed in situ NPD measurements of ceria,
which were carried out using iMATERIA(BL20) [9, 10].
The reduction of ceria at 800°C under hydrogen gas (3%H2 in N2) was investigated using an infrared gas furnace.
The oxygen pressure was less than 1022 atm. The ceria
pellets were placed in a quartz cell in the gas furnace.
After evacuating the air from the furnace, hydrogen was
injected at a gas flow rate of 50 ml/min. The heating/cooling rate was 10°C/min. The gas furnace was placedin an outer vacuum chamber and installed in the iMATERIA. In situ NPD measurements were performed at
isothermal holding time of 30 min. or 20 h between
800°C and 25°C. The crystal structure was analyzed using Rietveld refinement (Z-Rietveld: Ver. 1.0.2) [11, 12].

3. Results and discussion
A: Crystal structure analysis of the short holding time ceria
During the cooling process form 800°C to 25°C,
the new defined peaks of the sub-phase appeared
around the peaks of the main phase below 500°C. In
the results of Rietveld refinement at 25°C, the structure of the sub-phase was refined as the cubic oxyhydroxide CeO2H (CeIII) structure, as shown in Fig. 1. The
H atoms condensed around the O atoms, and the occupancy was 0.125 (32f site). The final result provided
the following crystallographic parameters for the cubic
structure (space group Fm-3m), for the main phase: a 
5.448319(8) Å, and for the sub-phase: a  5.51801(8) Å.
The mass fraction of the main phase and the sub-phasewere 93.1% and 6.9%, respectively. The lattice constantof the CeO2H crystal increased up to approximately
1.3% compared with that of the main phase. The expansion behavior correlated with the change in the ionicradius of Ce and also the incorporation of numerous H
atoms into the lattice.
B: Crystal structure analysis of the long holding time ceria
To evaluate the holding time dependence of thecrystal structural changes of ceria over 20 h at 800°C,
we sliced the isothermal holding time diffraction to thehourly measurement data, as shown in Fig. 2 (a). Thesediffraction peaks clearly showed that the d-spacing
shifting consists of high region for increasing the holding time. Figure 2 (b) shows the holding time dependence of the lattice constant for a holding time of 20 h.

Ce

H

O

c
a

b

Figure 1. Packing arrangement of the cubic CeO2H crystal.

59

MLF Annual Report 2018

The lattice constant continuously increased when theholding time was increased, because the extent of
Ce reduction tended to increase with the progress ofoxygen vacancy (the inset in Fig. 2 (b)). The 20 h data
were refined to a cubic oxygen-deficient structure. The
oxygen occupancy was estimated to be 0.9547(7), andthe corresponding composition was CeO1.909(1). Ceria assumed an oxygen-deficient structure after 3 h, and theoxygen deficiency continually increased until a holding
time of 20 h.
The temperature dependence of ceria during thecooling process between 800°C and 25°C is shown in
Fig. 3 (a). Additional peaks (sub-phase) with a low dspacing were seen as compared with the pattern of

4

5

6

7

8

9

10

11

12

13

14

15

16

17

18

19

20

(b)

30
25

5.53
20
15

5.52
10
5
0

200

422

1.92

1.93

111

15

10

1.94

1.95

1.96

1.97

1.98

d/ύ

CeO2−x
5.51

2.01
2
1.99

5.5

1.98

311

5.49

*

1.97
1.96
1.95
1.94
1.93

222

5

5.54

2-x@CeO2−x

3

220

2

Normalized intensity

20

1

400

Normalized intensity

25

220

30

(a)

the main phase at 500°C. Moreover, below 400°C, themain phase of ceria changed substantially to a completely different structure. At 500°C, the structures ofboth the main phase and sub-phase were refined as
cubic CeO1.892(1) and cubic CeO1.94(2), respectively. The
refinement of the data at 25°C revealed that the main
phase of ceria underwent a structural transition to thetriclinic oxygen-deficient structure Ce11O20 (i.e., CeO1.83)
as shown in Fig. 3 (b). Indeed, the structure of the subphase was entirely restored to CeO2. The final results
provided the following crystallographic parameters:(1) a main phase (Ce11O20), belonging to space group
P-1; (2) a sub-phase (CeO2), belonging to space group
Fm-3m.

Lattice constant /ύResearch and Development Highlights

1.92

*

1.91

5.48

**
*

1.9

CeO2
(CeO2Hy)

0

0

2

4

6

8

10

12

14

16

18

20

Isothermal holding time / hour

5.47
0

0.2 0.4 0.6 0.8 1 1.2 1.4 1.6 1.8 2 2.2 2.4 2.6 2.8 3 3.2 3.4 3.6 3.8 4 4.2 4.4 4.6 4.8 5

2

4

6

8

10

12

14

16

18

20

22

Isothermal holding time / hourd /ύFigure 2. (a) Time sliced in situ NPD patterns of ceria crystal during 20 h at 800°C. The diffraction of isothermal holding time at 20 h
was sliced to the 20 hourly measurement data (unit: h). Inset shows the diffracted patterns on 220. The asterisk denotes
the peaks of the thermocouple. (b) Isothermal holding time dependence of the lattice constants of ceria at 800°C. Inset:
time profiles of the 2−x value in CeO2−x during 20 h holding at 800°C.

(a)
25Υ

100Υ

(b)
Vo

Intensity / a.u.

200Υ
300Υ
400Υ
500Υ
600Υ
700Υ

c
b

800Υ

0.2

0.7

1.2

1.7

2.2

2.7

3.2

3.7

4.2

4.7

d /ύ

Figure 3. (a) NPD patterns of ceria crystal in the temperature range 25°C to 800°C. (b) Packing arrangement of the triclinic Ce11O20
crystal viewed perpendicular to the a axis. The black dot circle shows the oxygen vacancy (Vo) site.

60

MLF Annual Report 2018

C: Crystal transitions of ceria
At 800°C, the thermal diffusion and hydrogen incorporation into the lattice of ceria particle occur easily.
CeO2x was created by the desorption of water molecules from CeO2H. As cooling proceeded below 500°C,
the thermal was not propagated in the ceria lattice,and the incorporation of hydrogen might be difficult.
In particular, the “center” of the reduced ceria particles
was unstable, because of absence of reducing conditions. In order to oxidize from CeO2x phase to CeO2
phase, the CeO2x phase at the center/core of the ceria
particles underwent oxidation into CeO2 by accepting
oxygen from the outer region (outside) of the particles.
The CeO2 phase was concentrated at the center of theceria particle during cooling (CeIII ( CeIV ). On the other
hand, reduction of the outer phase of the ceria particles
was more pronounced in the bulk by desorption of the
O atoms from the particle. Strained Ce and O atoms of
the oxygen-deficient Ce11O20 structure were formed by
rapid breakage of covalent bonds at low temperature.
3. Conclusions
We investigated the crystal structure of ceria depending on the isothermal holding time at high temperature and various temperatures under hydrogen byusing in situ NPD measurements. In the case of short
holding time, the cubic oxyhydroxide (CeO2H) was
formed by the interaction of hydrogen interaction with

Research and Development Highlights

ceria during the cooling process from 800°C. On theother hand, the oxygen vacancies of ceria were kinetically progressed during a long holding time at 800°C.
Below 400°C, the main phase of CeO2x changed to a triclinic oxygen-deficient structure Ce11O20. The solid-gas
reaction of ceria occurred with strong dependence on
the isothermal holding time and the temperature.
References[1] Z. Hu, et al., ACS Catal., 6, (2016) 2265.
[2] S. P. Ray, et al., J. Solid State Chem., 15, (1975) 344.
[3] O. T. Sorensen, J. Solid State Chem., 18, (1976) 217.
[4] S. Bernal, et al., J. Chem. Soc. Faraday Trans., 89,(1993) 3499.
[5] K. Sohlberg, et al., J. Am. Chem. Soc., 123, (2001)
6609.
[6] B. Chen, et al., J. Phys. Chem. C, 117, (2013) 5800.
[7] X.-P. Wu, et al., Phys. Chem. Chem. Phys., 17, (2015)3544.
[8] K. Werner, et al., J. Am. Chem. Soc., 139, (2017)
17608.
[9] T. Ishigaki, et al., Physica B, 385–386, (2006) 1022.
[10] T. Ishigaki, et al., Nucl. Instrum. Meth. A, 600, (2009)189.
[11] R. Oishi, et al., Nucl. Instrum. Methods Phys. Res.,
Sec. A, 600, (2009) 94.
[12] R. Oishi-Tomiyasu, et al., J. Appl. Crystallogr., 45,(2012) 299.

T. Matsukawa, A. Hoshikawa, and T. Ishigaki
Frontier Research Center for Applied Atomic Sciences, Ibaraki University

61

Research and Development Highlights

MLF Annual Report 2018

Nuclear Magnetic Field Detected with μ±SR
1. Introduction
Positive muon spin rotation and relaxation (SR) isa unique technique to detect a nuclear magnetic field
in solids regardless of the presence of magnetic ions [1,2]. It provides a great advantage over NMR, particularly
for studying ion diffusion in cathode materials for a
Li-ion battery, because such materials always include
magnetic ions. Here, the implanted  sits at the interstitial site, where the electrostatic potential is minimal.
However, at high temperatures, such  starts to diffuse,
while one cannot predict the temperature above which becomes mobile. Therefore, the SR result obtained
at high temperatures unavoidably includes an ambiguity. We have therefore started a new project for detecting a nuclear magnetic field in solids with SR, since
the implanted  is captured on a nucleus, leading to
the formation of a muonic atom, which is stable even athigh temperatures.
Before measuring Li diffusion with SR, we haveattempted to measure the SR spectrum on MgH2
(Fig. 1), which was investigated extensively as a candidate of the hydrogen storage material, for detecting a
nuclear magnetic field. This is because, since the  captured on H in MgH2 is quickly transferred to Mg nuclei,
the SR spectrum is expected to be analyzed easily.

in the sample cell was monitored to know the change
in the SR parameters at the desorption temperature,that is, we have developed an in-situ SR technique [3].
The SR experiment on MgH2 was performed only
at room temperature in order to confirm the observationof a nuclear magnetic field. The experimental details forboth measurements are described elsewhere [3, 4].
3. Results
Figure 2 shows the temperature dependences ofthe field distribution width () and field fluctuation
rate ()) in MgH2 estimated with SR together with the

2. Experimental
The internal magnetic field in MgH2 was studied
with both SR and SR. During SR measurements
at temperatures between 300 and 800 K, the pressure

Mg
H

Figure 1. The crystal structure of MgH2 in tetragonal symmetry
with the space group P42/mnm together with the μ+sites predicted by DFT calculations [3]. The implanted μ+ distributes in a pinkish one-dimensional channel along the c-axs. On the other hand, μ− locates at
the Mg position. Reproduced from Ref. [3] with permission from The Royal Society of Chemistry.

62

Figure 2. The temperature dependences of the gas pressureand μ+SR parameters for MgH2 [3]: (a) gas pressurein the cell; (b) the field distribution widths (Δ1 andΔ2); (c) the field fluctuation rates (ν1 and ν2). Dipole
field calculations provide that Δcalc ranges 0.629 and0.664 μs−1. Dotted lines show the desorption temperature determined from the p(T) curve. Reproduced from Ref. [3] with permission from The Royal
Society of Chemistry.

MLF Annual Report 2018pressure (p) in the sample cell. Both  and ) are foundto be temperature independent below the vicinity ofthe desorption temperature (Td  680 K), around which
p increases very rapidly. Although SR shows a static
behavior up to 680 K, the magnitude of  is about 1/2 ofthe value predicted with dipole field calculations. Thisimplies the  diffusion in MgH2 above 300 K.

0.02
LF50 Oe
LF20 Oe
LF10 OeZF

A0P(t)

0.01

0

TF50 Oe

−0.01
0

MgH2
1

2

3

4

5

TIME (μs)
Figure 3. The TF-, ZF-, and LF-μ−SR asymmetry spectra for
MgH2 recorded at room temperature. The fit provides that Δ = 0.520(7) μs−1 [equivalent to a field
distribution width of 6.11(8) Oe], while dipole fieldcalculations predict Δcalc = 0.5807 μs−1 [6.819 Oe] at
the Mg site. Copyright 2018 American Physical Society.

Research and Development Highlights

On the contrary, SR provides a reasonable  forthe Mg site at room temperature (Fig. 3), as expected.
This demonstrates the unique power of SR for detecting an internal magnetic field in solids at hightemperatures.
4. Future plans
The nuclear magnetic field in MgH2 was successfully detected with SR from a fixed Mg position. Basedon this result, we wish to propose a combination of
SR and SR to obtain reliable information on the dynamic behavior in the nuclear magnetic field in solids.
Such combined work should be useful specifically formeasuring ion diffusion in battery materials and we areworking in that field.
References[1] J. Sugiyama et al., Phys. Rev. Lett., 103, 147601-1-4(2009).
[2] J. Sugiyama et al., Phys. Chem. Chem. Phys. 15,
10402–10412 (2013).
[3] J. Sugiyama et al., Sustainable Energy Fuels 3, 956–
964 (2019).
[4] J. Sugiyama et al., Phys. Rev. Lett., 121, 087202-1-5(2018).

J. Sugiyama1,2, I. Umegaki2, S. Takeshita3,4, A. Koda3,4, K. Shimomura3,4, and W. Higemoto3
Neutron Science and Technology Center, CROSS; 2Toyota Central Research & Development Labs., Inc; 3Muon Science Section, Materials andLife Science Division, J-PARC Center; 4Institute of Materials Structure Science, KEK

163

Neutron SourceNeutron Source

MLF Annual Report 2018

Progress of the Neutron Source Section
the same structure as target #8. The beam operation oftarget #9 had continued well at 500 kW with the highaverage availability of 93.2% as of the end of fiscal year
2018.
An important event was the transportation of
the used target vessel from the MLF (Materials andLife Science Experimental Facility) to the RAM (Radio
Activated Materials) building to save the limited spaceof the used components storage room in the MLF. A
shielding container, 200 mm in wall thickness and 44
tons in total weight, was fabricated and used in combination with the shipping container fabricated in 2017. The
preparation and rehearsal took almost a month and theused target vessel was transported successfully to theRAM building for the first time on January 16, 2019. The
transportation is going to be held every year.

0.8
Displacement velocity [m/s]Fiscal year 2018 started with a beam operation of
500 kW, which had been recognized as an importantmilestone to reach the final goal of 1 MW. Since twotargets failed consecutively during the 500-kW beam
operation in 2015, considerable efforts were put into
improving the design of the next mercury target, target#8, to make it more robust and reliable in a high-power operation. Target #8 had been used at 300 kW and
400 kW since the last fiscal year and completed its user
beam operation successfully on June 30, 2018 after a
3-months operation at 500 kW, which demonstrated thevalidity of the design improvement. Additionally, target#8 was operated with a 935-kW power for one hour at thehigh-power beam study held on July 3. Reaching almost
1 MW was a great achievement for J-PARC.
Gas-micro-bubbles injection into mercury and thehigh-speed mercury flow in a narrow channel formedby the double walled structure, shown schematicallyin Fig. 1, are the key measures to mitigate the pitting
damage at the beam window located at the front endof the target vessel. At the high-power beam study, thevibration of the target vessel under the beam operation
condition of 25 Hz was measured at almost 1 MW for the
first time, as shown in Fig. 2. The displacement velocity
on the top side of the target vessel at 935 kW remainedon the same trend line with those measured at a lower
beam power. It shows the efficacy of gas-micro-bubble
injection to reduce the displacement velocity at a 1-MW
operation.
The specimens were taken out of the used target#8 and the maximum depth of pitting damage on the
inner side of the beam window was 18 m, which wasless than predicted. This fact demonstrated the effectiveness of the present measures to mitigate pitting damage.
Then, target #8 was replaced with target #9, which has

0.7
0.6
0.5
0.4 W/O micro-bubbles
0.3
0.2

With micro-bubbles

0.1
0

0

200

400
600
Beam power [kW]

800

1000

Figure 2. Displacement velocity at the top side of target
vessel #8 at beam study.

Protonbeam

Hg
Double walled

Swirl bubbler

Figure 1. Measures to mitigate pitting damage applied intarget #8.

K. Haga
Neutron Source Section, Materials and Life Science Division, J-PARC Center

66

Shipping container
Figure 3. Transportation of a used target vessel.

MLF Annual Report 2018

Neutron Source

Operation Status and Design Improvement for the
Mercury Target Vessel
1. Introduction
In a mercury target for the J-PARC neutron source,
reduction of the pressure waves caused by rapid thermal
expansion of liquid mercury due to the high-intense
pulsed 3 GeV proton beam injection at 25 Hz is a key
to achieve high-power stable operation. The pressure
waves induce not only fatigue but also severe cavitation
erosion on the mercury enclosure vessel [1]. To reduce
the pressure waves, the mercury target system has been
operated with helium microbubbles injection into mercury by using cushion effect of the microbubbles [2].
Here, the operational result of target vessel No. 8
is reported, which was operated under gas microbubbles injection into liquid mercury to reduce the pressure
waves. Furthermore, an improved target vessel design
to reduce thermal stress for the high-power operationis also introduced.
2. Gas microbubble injection
In the original operation, helium gas, pressurized
by a compressor, was supplied to the bubble generator
which made a crowd of gas into microbubbles. Since
December 2017, the gas has been supplied to the bubble generator without an operating compressor becauseof the possibility that the activated gas could spill into
the environment in the case of compressor failure under
the high pressure of 300 kPa.
To avoid high pressure in the gas-supplying line during operation, the configuration of the bubble generator
was improved to create negative pressure at the bubbler
and bring in an amount of gas comparable to the one
delivered when the compressor was still used. During
the operation, the vibration of the target vessel due tothe pressure waves was monitored by a Laser Doppler
Vibrometer to understand the reduction behavior of thepressure waves changed by gas microbubbles injection.
Figure 1 shows the time histories of the peak amplitude of vibration (displacement velocity) on target
vessel No. 8 and the beam power. As the beam power
was ramped up from 300 kW to 400 kW, the velocity
increased from 0.13 m/s to 0.17 m/s. The estimated displacement velocity without microbubbles [1] is also
shown in Fig. 1. The ratio of the measured displacement
velocity to the estimated one without microbubble isapproximately 0.3, which is independent of both thebeam power and the operation with or without compressor. In short, the amount of microbubble injection
for improved bubble generator without compressor was
as much as with the operating compressor.
3. Effect of the gas microbubble injection on
cavitation damage
The beam window portion of the used target vessel
No. 8, which operated at up to 1812 MWh and 434 kW inaverage power, was cut using an annular cutter aiming
to investigate the effect of a gas microbubble injection
into the mercury. Figure 2 shows the photographs of theinterior surface cutout from the used target vessel. It canbe seen that the localized deep pits are recognized on the
inner wall surface facing the bubbly mercury, whereas thepits with lesser damage are recognized on the outer wall
surface facing the narrow channel. The cavitation damageon the narrow channel surface was slightly less than thatof the damage observed in target vessel No. 5 that was
operated under the average beam power of 400 kW. The
max. damage depth of the inner wall surface was estimated to be 286 m. It was found that the estimated damage
depth faced with bubbly mercury was corresponded tothe damage formed at approximately 30% of the beam
power without injecting gas microbubbles [2, 3].
Dmax:17.5 μm.

Dmax:286 μm
.

1 mm

1 mm

10 mm

Figure 1. Time history of displacement velocity on target vessel No.8 and the beam power.

Outer wall

Inner wall

Figure 2. Cutout surfaces of target vessel No. 8.

67Neutron Source

MLF Annual Report 2018

4. New target vessel, constraint free type, design
and fabrication
Figure 3 shows a schematic cross-sectional view ofan improved mercury target vessel. A mercury vessel iscovered by a water shroud to prevent spills of mercury
in a case of its failure. The original design of the mercury target vessel had a constraint structure between
the water shroud and the mercury vessel with monolithic structure to maintain the robustness as shownin Fig. 4(a) [4–5]. The structure of the vessels has been
greatly improved from target vessel No. 10. In particular, the constrain free structure between the mercury
vessel and the water shroud was adopted to reduce thethermal stress during high-power operation in addition
to improve the location of welding line and fabrication
process (Fig. 4(b)) [6]. As seen in the figure, the mercury
vessel and the water shroud is fixed at the end of themercury vessel through a support plate by TIG welding. The main design conditions of the target vessels
are shown in Table 1. In the constraint free type design,
it is expected to reduce the thermal stress due to thedifference of thermal expansion between the mercury
vessel and the water shroud, whereas the deformation

Figure 3. A cross section view of mercury target vessel. The
support plate is shown in the left-hand side.

(a)

(b)

Figure 4. Schematic cross-sectional images of (a) a constraint
structure and (b) a constraint free structure between mercury vessel and water shroud.

Table 1. Design condition of mercury target vessel.
Design Pressure (MPa) Temperature of inlet (°C)
Hg (Layer)
He (Layer)
H2O (Layer)

0.5
0.2*0.2 or 0.5

50
25
25

*0.5 MPa for #11, and #12, 0.2 MPa for #8, #9, and #10

of water shroud by the gas pressure in the helium layer
is increased. Therefore, it was necessary to modify somedesigns for the fabrication technique and processes,
such as water channels, support plate structures, andwelding technology using electron beam welding.
The calculated thermal stress decreased and was
improved in comparison with the previous type. The
new type has been fabricated, and it will be operated
from December 2019.
5. Summary
1) The peak vibration (displacement velocity) on target
vessel No. 8 was evaluated under the beam powerof 300 and 400 kW. The ratio of the measured velocity to the estimated one without microbubble wasapproximately 0.3, which was independent of bothof the beam power and the compressor operation.
2) The beam window portion of the used No. 8 was
cut to investigate the effect of the gas microbubble injection into the liquid mercury. The cavitation
damage on the narrow channel surface was slightly
less than that of No. 5, and the max. damage depthof the inner wall surface was 286 m.
3) New target vessel with constraint free type was designed and fabricated.
References[1] T. Naoe, et al., Cavitation damage prediction for
the JSNS mercury target vessel, J. Nucl. Mater. 468(2016) 313–320.
[2] H. Kogawa, et al., J. Nucl. Sci. & Tech., 54 (2017)733–741.
[3] H. Kogawa, et al., J. Nucl. Sci. & Tech., 52 (2015)
1461–1469.
[4] T. Wakui, et al., J. Nucl. Mater. 506 (2018) 3–11.
[5] T. Wakui, et al., presented in IWSMT14, in Iwaki,
Japan (Nov. 2018).
[6] E. Wakai, et al., Proceedings of the 15th annual
meeting of Particle Accelerator Society of Japan,(2018) 181–184.

E. Wakai1, H. Kogawa2, T. Naoe2, and T. Wakui2
Materials and Life Science Division, J-PARC Center; 2Neutron Source Section, Materials and Life Science Division, J-PARC Center

1

68

MLF Annual Report 2018

Neutron Source

Quadrupole Magnet (QC12) Trouble in 3NBT
1. Introduction
The 3-GeV proton beam transport facility (3NBT)
transports the beam from the 3-GeV Rapid Cycling
Synchrotron (RCS) to the Material and Life Science
Experimental Facility (MLF) in J-PARC. In the 3NBT, the300-meter long beamline has many electric magnets
such as 9 bending, 54 quadrupole, 48 steering, and 2
octupole magnets. Here we report a failure of a quadrupole magnet (QC12, see Fig. 1) that happened on May
17, 2018.
2. Failure of the magnet
At 4 AM on May 17, 2018, a layer short occurred at
the coil of quadrupole magnet QC12. The layer shortcaused an unbalanced quadrupole magnetic field.
Along the downstream of the QC12, the beam position moved into the horizontal and vertical directions.
By the beam orbit confirmation, the beam was kickedat the QC12 with an angle of about 7 mrad for both
directions. This angle was created by the offset of thecenterfield 7 mm to the magnet. When the layer short
happened, the beam position shifted about 40 mm in
the vertical direction at the beam monitor placed at
the proton beam window (PBW). The beam shift led

to an abnormal temperature increase, which was observed by the beam halo monitor placed at the PBW.
Eventually, the machine protection system (MPS) of thebeam halo monitor stopped the beam.
The quadrupole magnet is driven by the given current to control the field. Due to the layer short, the supplied voltage dropped from 77 to 71 V. Several hours
after the event, the supplied voltage was stable, which
implied conserving the status. Therefore, we decided
to continue the beam operation by using steering
magnets to centralize the beam position. As a countermeasure against further layer short, we added theinterlock for the beam position and the current densityof the beam monitors placed at the PBW. Also, the interlock was added for the supplied voltage of QC12. Afterbeam tuning and additional interlock, the beam operation resumed successfully 13 hours later at 5:15 PM.
3. Research of the layer short
Figure 2 shows a cross-sectional view of the QC12
coil. Each coil has 129 turns of a hollow conductor
made of dioxide copper. Due to the flow of the cooling water with the temperature kept less than 60°Ctoprevent erosion, the coil was divided into three zones

Figure 1. Segment of the 3NBT proton beamline from around QC12 to the neutron target.

Figure 2. Overview of the QC12 coil (left) and cross-section of the A-A’ and B-B’ position.

69

Neutron Source

MLF Annual Report 2018

Figure 3. Photo (on the left) and infrared image (on the right)of the QC12. The infrared image shows a normal
coil and a coil with short circuit.

called inner, middle, and outer coil. The reactance andinductance of the coil were measured for each zone.
The inductance of the inner coil and middle coil was
found to be about one-tenth of the others. It was concluded that the layer short occurred between the innerand middle coil. In order to find the anomaly coil, weobserved the temperature distribution of the coil withan exciting magnetic field. Figure 3 shows the infra-red
image of the QC12. It was found that the coil placed at
the lower part showed lower temperatures than otherones, which did not have layer short. The infra-red viewalso suggested that the layer short happened between
the inner and middle coil, even though it was difficult to
pinpoint the exact place of the short circuit.
4. Subsequent actions
There was a possibility for the layer short to worsen
over a longer time period. Although we had a spare coil,the exchange of the coil for the QC12 was expected totake long, about one month. In order to replace the coil,
we had to take an unscheduled beam stop. Therefore,
we tried to find the solution without the usage of the
QC12. After beam study, we found a solution of thebeam optics that excluded the affected magnet but
prevented significant beam loss. Without the use of the
QC12, the beam operation continued until the summer
outage period. It should be mentioned that the demonstration with a 1-MW beam power was made without
the use of the QC12. Since the beam quality of the Rapid
Cycling Synchrotron (RCS) was better than designed, ahigh-intensity beam operation was completed without
the QC12 successfully without beam loss.
Although the cause of the layer short has not been
determined yet, it was probably related to a water leak
event in the early days of the QC12 magnet. The waterleak may cause corrosion with the radiation leading to
the layer short. Since another quadrupole magnet had
leaked water in the past, it was decided to exchange thecoil in the next year as a precaution against layer short.
Furthermore, in order to apply quick recovery against
more layer shorts in the future, a study without the usage of another quadrupole magnet will be performed
later.
It should be noted that the method of deactivating
the magnet can be applied for the quadrupole. For thebending magnet failure, the coil must be exchanged. In
2019, the bending magnet for the beam transport fromthe RCS to the 30-GeV synchrotron (MR) failed. The lackof a spare coil for the failed magnet halted the beam
operation of the MR for a long time. All of magnet failure events were somewhat related to the corrosion of
the coil. To avoid the corrosion, the purification systemof the cooling water will be improved. Also, the failure
event showed the importance of having a spare coil.
Therefore, we will increase the number of spare coils tohandle effectively the failures of the magnet.

M. Ooi and S. Meigo
Neutron Source Section, Materials and Life Science Division, J-PARC Center70

Neutron ScienceNeutron Science

MLF Annual Report 2018

Neutron Science Section
1. User program
In the beginning of JFY2018, the target was operated at 400 kW and from April 19, the power was increased up to 500 kW.
For the general-proposal round for 2018A, 175 general proposals and 5 new user promotion (NUP) proposals were approved from 260 submissions. 174 approved
experiments and 9 reserved ones were executed
among them. For 2018B, 190 general proposals and 8
NUP proposals were approved from 285 submissions.
178 approved experiments and 13 reserved ones were
executed among them. Additionally, 4 newly approved
long-term proposals became the beginning of a 3-years
project from 2018B term. Fast Track Proposal, which
is a mail-in program, has just started from the end of
JFY2017 for Super HRPD at BL08 and NOVA at BL21. In
2018, 3 experiments were executed at BL08 and 2 experiments were done at BL21.
2. Instruments
The layout of the neutron instruments at the MLF,
as of the end of JFY2018, is shown in Fig. 1.
This year, the MLF was stably operated with beam
power of 500 kW . On July 3, a test operation with
1 MW was performed for 1 hour. The high beam power
was experienced in each beam line. For example, on
the chopper spectrometers AMATERAS at BL14 and
4SEASONS at BL01, inelastic neutron scattering from S 

Figure 1. Layout of the neutron instruments at MLF as of
JFY2018. BL23 was in the commissioning phase.

72

1/2 one-dimensional antiferromagnets were measured.
The dispersion relation of the spin excitations could be
identified in the measurement for a few minutes, andwell-analyzable data were obtained even within 1 hour.
Since the start of the user program in the MIEZE
part of the neutron spin-echo suit VIN ROSE at BL06 in
2018, scientific outcomes are starting to appear. An experiment was performed in MnSi, where various spin
structures, such as helical spin structure, conical spin
structure, and skyrmions, are expected below the transition temperature. Clear spin relaxation was successfully observed just above the transition temperature.
POLANO (Polarized Neutron Spectrometer) at BL23
is still under commissioning. On-beam commissioning
using actual samples was performed with an unpolarized neutron beam. Magnetic excitations in a singlecrystalline sample of one-dimensional antiferromagnet
CsVCl3, whose excitation energies spread up to 80 meV,were successfully observed. Also, excitations in ZrH2
were observed. In ZrH2, the motion of a hydrogen atom
can be approximated to be a quantum harmonic oscillator, and energy levels with an equal interval can beobserved. Using the detector system covering scattering angles up to 130°, the entire S(Q, ω) of the harmonic
oscillator was clearly observed. These results indicatethat POLANO is useful not only for studies of spin systems but also for studies of hydrogens. POLANO will
open for user program from 2019A with unpolarized
neutrons.
3. Event, meetings, and other activities
The 3rd Neutron and Muon School was held in
November 20–24. 35 young researchers and graduate
students from China (8), India (5), Korea (1), Thailand (1),Russian Federation (1), United Kingdom (1), as well asJapan (17) participated in the school. From the neutrongroup, 9 neutron instruments (4SEASONS, DNA, iBIX,PLANET, TAKUMI, iMATERA, TAIKAN, SHARAKU) were
contributed to hands-on experiments (Figs. 2 and 3).
J-PARC Center and CROSS hosted the J-PARC
Workshop “Deuterium Labeling Study for Neutron
Science” on January 15 and 16, 2019. We invited Dr. T. A.
Darwith from ANSTO and the 20 participating scientists
discussed neutron studies on material and life siences
by utlizing deuterium labeling.
The neutron science group hosted user groupmeetings of individual intruments. DIRECTION 2019
(MLF spectroscopy group user meeting) was held on

MLF Annual Report 2018

Neutron Science

Scattering Association (AONSA), we accepted as a research fellow Dr. Xingxing Zhang (Institute of Metal
Research, Chinese Academy of Sciences). Dr. Zhang
joined TAKUMI group from November 1 to December
27 and he enjoyed his research on Al-based composit
materilas.

Figure 2. Dr. Kosuke Hiroi explaining the operation of the
shutter control pannel at TAIKAN at the 3rd Neutronand Muon School hands-on experiment.

4. Resultant outcomes
The research activities in neutron science at the
MLF resulted in more than 180 papers and 10 press
releases. The number of papers includes articles in
influential journals such as Nature Physics (1), Nature
Materials (1) and Scientific Reports (6). Press releases
included two detector developments, such as a highresolution (11 nm) emulsion type detector and ahigh-speed neutron imaging detector via a solid-statesuperconducting detector.
Dr. Takuro Kawasaki won the 16th Young Researchers Prize of the Japanese Society for Neutron
Science for the development of stroboscopic measurements and leading research with the technique on
SENJYU (BL18) and TAKUMI (BL19).
The RADEN (BL22) group won JAEA President’sAward for the development of energy-resolved neutron
imaging and leading researches on RADEN.

Figure 3. Dr. Shinichi Takata explaining instruments in the experimental hall of MLF to students of the 3rd Neutron and Muon School.

October 11 at Ibaraki Quantum Beam Research Center(IQBRC). We had 54 participants. User group meetingof DNA was held on October 12 at IQBRC and 18 particpants joined. We also had user group meeting of
RADN (October 10) and PLANET (October 11). At thesemeeting, latest information of instruments and recent
outcomes from experiments by users were presented
and the users provided feedback to the instrumental
scientists.
In the frame work of the young research fellowship program orgnaized by the Asia-Oceania Neutron

Figure 4. Dr. Takuro Kawasaki recieving certification fromProf. Y. Kiyanagi, the president of the Japanese Society for Neutron Science.

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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MLF Annual Report 2018

BL01: 4D-Space Access Neutron Spectrometer 4SEASONS
1. Introduction and statistics
4SEASONS is a direct-geometry time-of-flightneutron spectrometer for thermal neutrons, and oneof the Public Beamlines in MLF [1]. The momentumenergy region for this spectrometer occupies the middle of the momentum-energy space covered by all
the MLF spectrometers [2, 3]. In 2018, 23 General Use(short-term) proposals, 1 Project Use proposal, and 1
Instrument Group Use proposal, were approved for
4SEASONS. In addition, 1 reserved (short-term) proposal was given beamtime. About 80% of the proposals were submitted for the fields of magnetism andstrongly correlated electron systems. 2/3 of the proposals targeted magnetic excitations, while 1/3 of the
proposals were for measurements of phonons. As forthe outcomes from using the instrument, 15 peer-reviewed papers were published in 2018. 12 were papers
for material science, while 3 papers were related to the
instrumentation.

Based on the results of an investigation of the straymagnetic fields by calculation and an operation test
without neutron beam, we performed an on-beamdemonstration of the magnet this year [5]. For thisdemonstration measurement, we employed a single
crystal of TbB2C2. A previous inelastic neutron scattering study using a powder sample of TbB2C2 reported
that magnetic excitation appears around 3.5 meV at
low temperatures, and it shifts toward higher energies
under applied magnetic field (H) of the order of 1 T [6].
Figure 1 shows the magnetic excitation spectra measured under H  3 T. The data were powder-averaged
and sliced in the range of Q  1.5–2 Å1. At H  0 T, weobserved a broad excitation peak around 3 meV. As H
increased, the peak sharpened and changed its position toward higher energies. These observations reproduce well the results in Ref. [6].

74Intensity (arb. units)

1.4
2. Instrument upgrade
Detectors: 4SEASONS is equipped with a number of3/4 inch  2.5 m 3He position sensitive detectors. We
have been increasing the number of detectors since
the start of the instrument’s operation. In 2018, we installed 37 detectors. As a result, the maximum scattering angle in the horizontal plane reached 127 degrees.
Fermi chopper: We have been developing a Fermi
chopper with supermirror-coated slits, which is expected to provide higher transmission at low energies. In 2014, we conducted a performance test of a
prototype, which this year was finally followed by aperformance test of a real model. We expected the realmodel to perform better than the prototype, because
the supermirrors used in the real model have higher reflectivity. We found that the real model showed higher
transmission at a high-energy region. Unexpectedly,
however, the transmission at low energies was lower
than that with the prototype. We suspect the supermirror does not work as expected, but the true cause
is still unclear.
Sample environment: There are difficulties in theuse of the high-field magnetic device at 4SEASONS,
because the instrument consists of many iron components. Because of that, we have investigated whether
the superconducting magnet of the MLF Sample
Environment Group can be used at our instrument [4].

1.2
1.0
0.8
0T
1.5 T
2.2 T
3T

0.6
0.4
1.5

2

2.5

4
3
3.5
Energy (meV)

4.5

5

Figure 1. Powder-averaged inelastic neutron scattering profiles of Tb11B2C2 at 4 K as a function of energy transfer. Open circles, closed circles, open squares, andclosed squares denote the data measured under0, 1.5, 2.2, and 3 T, respectively. The solid lines are
guides to the eye [5].

Acknowledgements
We thank H. Kira, K. Kaneko, S. Ohira-Kawamura, R.
Takahashi, K. Aoyama, and W. Kambara for their support and advice. The instrumentation works describedhere were supported by the engineers of the Neutron
Science Section and the Technology Development
Section of MLF.

MLF Annual Report 2018

References[1] R. Kajimoto et al., J. Phys. Soc. Jpn. 80, SB025 (2011).
[2] H. Seto et al., Biochim. Biophys. Acta, Gen. Subj.
1861, 3651 (2017).
[3] R. Kajimoto et al., Physica B 562,148 (2019).

Neutron Science[4] R. Kajimoto et al., J. Phys.: Conf. Ser. 1021, 012030(2018).
[5] R. Kajimoto et al., Physica B 556, 26 (2019).
[6] A. M. Mulders et al., Physica B 359–361, 1231
(2005).

R. Kajimoto1, M. Nakamura1, K. Kamazawa2, Y. Inamura1, K. Ikeuchi2, K. Iida2, M. Ishikado2, and N. Murai1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science and Technology Center, CROSS

1

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MLF Annual Report 2018

Current Status of BL02 DNA in 2018
1. Introduction
DNA is a TOF backscattering spectrometer designed to elucidate atomic and molecular dynamics [1].
DNA can provide micro-eV energy resolution measurements over a broad energy range of 500 eV E
1500 eV, thanks to the near-backscattering geometry of the instrument and its pulse-shaping options.
In addition, back-coated Si analyzers with Gd or Gd2O3
neutron absorber give extra high signal-to-noise ratioof around 105, which enables to detect small scattering
amplitudes or signals from small quantities of samples.
The accessible momentum transfer range is from 0.08
to 1.86 Å1 by using Si111 analyzer mirrors.
The number of peer-reviewed papers from DNA
was 9 in 2018 almost the same number (8) as in 2017 [2].
2. User Program in the periods 2018A and 2018B
11 General Proposals (GP) including 1 New User
Promotion (NUP) proposal, and 10 GPs including 2
NUP were approved for 2018A and 2018B, respectively.
The portion of approved beamtime from all requested
beamtime was 63% for 2018A and 40% for 2018B. The
competition rate of 2018B, 2.3, was much higher than
1.2 for 2018A. Additionally, two reserved proposals
were also conducted in 2018B.
Also, on the General Proposal (Long Term) (hereafter LTP) Program, two proposals have been newly
adopted from 2018B. In total, three LTP’s run at BL02.
The 3rd Neutron and Muon School was held in
November. We accepted 4 students. They enjoyedhands-on experiment on molecular dynamics of waterin Nafion membranes at DNA.

6

(a)

-1

Q = 0.2 Å
300 Hz 1cm-1cm
FWHM=1.4 μeV
225 Hz 1cm-1cm
FWHM=1.6 μeV

5

S (Q,E) /a.u.

4

3. Beamline activities
Beamline
The fast disk choppers used in DNA showed vibration at high speeds, which limited the maximum available speeds to 225 Hz. In January 2019, improved disks
were installed, which made it possible to achieve thedesign speed of 300 Hz. We found that the best energy
resolution using 10 mm slit with 300 Hz was 1.4 eV for
10 mm tall sample, which confirmed the design valueof DNA (Fig. 1(a)). The improvement was also remarkable for the 30 mm slit, the most frequently used condition in entire Q-region, as shown in Fig. 1(b).
On July 3, 2018, MLF succeeded in operating continuously for one hour at a beam power of approximately
1 MW. Test measurements were performed to demonstrate the performance of DNA at 1 MW. Figure 2(a)shows the temperature dependence of the elastic intensity of starch with water. Clear drops at 0°C were observed
for all data, whereas the drop at 60°C appears only forthe first heating data due to gelatinization, which confirms the change obtained by differential thermal analysis with the same heating/cooling speed of 1°C/min.
Figure 2(b) shows QENS spectrum with a measurement
time of 2 minutes at 50°C during the heating process.
The quality of the spectra was enough for quantitative
QENS analysis. Thus, a beam power of 1 MW enables thestudy of dynamics in conditions nearly identical to thoseof a typical thermal analysis. Conventional QENS measurements have been limited to thermally-equilibrated
systems. High-intensity neutron beams will open a newarea of innovative application of QENS to the non-equilibrium phenomena, such as the starch gelatinization.

(b)

3
2
1
0
-6

-4

-2

0

2

4

6

ΔE / μeV

Figure 1. (a) Best energy resolution before (225 Hz) and after (300 Hz) installation of the new fast chopper disk with
1 cm-1 cm slit. (b) Q-dependence of the energy resolution with 3 cm-3 cm slit.

76MLF Annual Report 2018(a)

Neutron Science(b)

Figure 2. (a) Temperature dependence of the elastic intensity of starch with water measured at a beam power of approximately 1 MWwith heating and cooling rate of 1 degree/min. (b) QENS spectrum at Q = 1.0 Å−1 with time bin of 120 seconds at 50 degrees.

Eight years have passed since starting the operation of DNA, and now we found problem of the beam
monitor caused by aging. The intensity of the beam
monitor was gradually reduced by a half between 2013
and 2017. Therefore, we replaced the monitor to a fresh
monitor in January 2019. Since, in DNA, we normalize
the scattered intensity by spectra of the beam monitor
installed before the sample, the stability of the beam
monitor is crucial. We plan to refresh the converter gas
for the old monitor.
Sample environment
Owing to the variety of samples measured at DNA,
experiments using special sample environments, suchas dilution refrigerator, magnet, high-pressure cell,sample changer, and vapor-controlled system, have increased in number at DNA. To meet their requirements,
we have installed distribution boards of electricity,cooling water, and He gas on the roof shield of DNA. In
addition, a part of the fence surrounding the roof waschanged to a sliding type to easily bring apparatus fromthe ground level onto the roof shield.
Software
The software package Utsusemi has been customized to reduce and visualize data from DNA. On the other hand, such customization prevents us from keeping
up with the modification of Utsusemi. We have incorporated DNA’s special code into the latest Utsusemi.

4. Future plans
Si311 analyzer mirrors extending the momentum
transfer range to 3.8 Å1 with 12 micro eV resolution
with 10 mm slit will be installed in 2019–2020.
5. Others
In 2018, DNA joined the user group meeting on the
MLF spectrometers “DIRECTION 2018” held on October
11 in Tokai. 54 attendees discussed new science andmethods obtained from the MLF spectrometers. After“DIRECTION 2018”, we had the first user group meetingfor DNA on October 12 with 18 attendees. The current
status and future plans of DNA, including the development of sample changer, auto gas-exchanger, fitting
program (QENS fit), and data correction, were shown by
the instrument team of DNA. In addition, we had extensive discussions on the future plans for neutron studies
in biology, the current status of software development
at MLF, and requests from users.
We had a guest, Mr. Shun Asano as an intern-student from Tohoku University in January of 2018. He
studied measurement and analysis of quasi-elastic scattering at DNA. He also participated in the commissioning of the improved fast disk chopper.
References[1] Kaoru SHIBATA et. al., JPS Conference Proceedings,
8 (2015), 036022.
[2] Ryoichi Kajimoto et. al., Physica B: Condensed
Matter, 562 (2019) 148.

Y. Kawakita1, M. Matsuura2, T. Yamada2, T. Tominaga2, M. Kobayashi2, and H. Nakagawa1,3
1Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science and Technology Center, CROSS; 3Materials
Sciences Research Center, JAEA

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MLF Annual Report 2018

IBARAKI Biological Crystal Diffractometer iBIX
1. Introduction
The IBARAKI biological crystal diffractometer iBIX
was constructed to perform high throughput singlecrystal neutron structure analysis, mainly for biologicalmacromolecules in various life processes at BL03, MLF(2008) [1]. To achieve high performance, we developed
successfully, in cooperation with JAEA, a new photoncounting two-dimensional detector system using
scintillator sheets and wavelength-shifting (WLS) fiber
arrays for the X/Y axes. In 2012, the installation of 30 detectors on the iBIX diffractometer was completed [2]. By
the end of 2012, iBIX became available for user experiments on biological macromolecules, supported by the
Frontier Research Center of Applied Atomic Sciences,
Ibaraki University. The final specifications of iBIX areshown in Table 1.

Table 1. Specifications of iBIX.
Moderator

CoupledWavelength of incident neutron (Å)

0.7 ~ 4.0 (1st frame)
4.0 ~ 8.0 (2nd frame)

Neutron intensity (n/s/mm2)(@1 MW)

0.7 × 106

L1 (m)40

L2 (mm)491

Solid angle of detectors (% for 4 )22.0

Detector covered region (deg.)

15.5 ~ 168.5

2

Detector size (mm )133 × 1332

Detectors pixel size (mm )0.52 × 0.52

No. of detectors

34

2. Current status
In 2016, we carried out neutron structure analysis
of Mn Catarase with the largest unit cell in the neutron
diffraction experiment by using iBIX to estimate its own
performance. The results showed that iBIX was able
to achieve the maximum cell dimension of the design
specifications without any peak de-convolution procedure. And then, it was confirmed that iBIX achieved alldesign target values (maximum cell dimension, resolution, measurement efficiency, etc.). In 2017, we assembled by ourselves the four newly added detectors. They
have already been installed on the iBIX diffractometer(Fig. 1). The measurement efficiency with 34 detectors
will increase 1.13 times over that of the previous 30
detectors. Commissioning the without/with neutron
78

Figure 1. The current diffractometer iBIX.

beam has already finished. By using the four newly added detectors, we could obtain the TOF diffraction datawith the same accuracy as with the current detectors.
The new detectors are available for users experiments.
In 2018, J-PARC was operated regularly at accelerator power of 500 kW. The results from the experimentson the full data set of biological macromolecules forneutron structure analysis by using iBIX were as follows. We were able to collect a full data set of biological macromolecules for neutron structure analysis witharound 2.0 Å resolution in about 8 days by using iBIX
at accelerator power of 500 kW. The average volumeof the sample measured by iBIX was about 1.5 mm3. If
the accelerator power reaches 1 MW, the total measurement time of the sample size will be reduced to a halfof the previously necessary time or the sample size canbe reduced by a half with the same measurement time.
We prepared a users’ manual and a distribution
package of the data reduction software “STARGazer”,
which would allow the iBIX users to perform personallydata reduction in their laboratory [3]. STARGazer works
on Linux and on Windows and OS X with virtual box.
We continue to develop the data reduction software inorder to improve its usability.
3. Future plans
We assumed that a full data set of a 2-mm3 protein
sample could be obtained by iBIX in about 2 to 4 days
under the 1-MW operation. The assumption impliedthat iBIX was capable of achieving the designed target
value. However, the sample size was still large, and themeasurement time was still long, especially for the users. We would like to reduce the difficulties of sample

MLF Annual Report 2018

preparation as much as possible. In other words, it isnecessary to further improve the measurement efficiency of iBIX by developing the beam line instrument.
As a simple and effective way to improve the measurement efficiency, we carried out the installation of
the newly added detectors. A maximum of 60 detectors can be installed on the support frame of the iBIX
diffractometer without any design changes. We will try
to get a construction budget to install the additional
detectors. Currently, we also consider other possibilities to improve the measurement efficiency. For example, increasing the beam divergence by the insertionof a super mirror, changing the distance between thesample and the detector surface, improving the chopper instrument, and so on. We will continue to develop
both the data reduction software and the beam line

Neutron Science

instruments to improve the measurement efficiency
and the accuracy of the intensity data obtained fromsmaller protein samples in order to build a single-crystal neutron diffractometer for biomacromolecules with
one of the highest levels of performance in the world.
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.
[3] N. Yano, T. Yamada, T. Hosoya, T. Ohhara, I. Tanaka
N. Niimura and K. Kusaka, Acta Cryst. D74 (2018)
1041–105.

K. Kusaka1, T. Yamada1, N. Yano1, T. Hosoya1, I. Tanaka1, and T. Ohhara2
Frontier Research Center for Applied Atomic Sciences, Ibaraki University; 2Neutron Science Section, Materials and Life Science Division,
J-PARC Center

1

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MLF Annual Report 2018

Neutron Total Cross Section Measurement at ANNRI(BL04)
1. Introduction
Accurate data of neutron-capture cross sections areimportant in detailed engineering designs and safety
evaluations of innovative nuclear reactor systems.
Especially, nuclear data for minor actinides (MAs) andlong-lived fission products (LLFPs) are necessary forburn-up analyses of nuclear fuels, improving the design
and performance of advanced nuclear reactors and thenuclear transmutation [1]. However, accurate measurements of these cross sections are very difficult to obtain
due to the high radioactivity of these samples.
To satisfy these demands, a time-of flight experimental instrument named “Accurate Neutron-Nucleus
Reaction measurement Instrument (ANNRI)” has been
constructed by the collaboration of Hokkaido University,
Tokyo Institute of Technology, and Japan Atomic Energy
Agency. Measurements of neutron-capture cross sections of MAs, LLFPs and some stable isotopes with highintensity pulsed neutrons have been started in 2008 [2].
In recent years, a measurement system for neutron total
cross section has been developed and the first results ofthe total cross sections were reported.
2. Detectors and DAQ
For neutron total cross section measurements, twotypes of Li-glass scintillation detectors have been installed in ANNRI. The set-up of the detectors is shownin Fig. 1. A 6Li-glass detector (PMT:H7195) manufactured by OKEN has been installed at flight length of
28.7 m to obtain transmission neutron TOF spectra.
The scintillator of the detector is GS-20 manufactured

Figure 1. The photo and the schematic view of the Li-glass
detectors for total-neutron cross section measurement.

80

by Saint Gobain with dimensions of 50 mm  50 mm
and a thickness of 1 mm using enriched 6Li (6Li enrichment higher than 95%). Neutrons passing through thesamples are detected by the 6Li-glass detector via the
6Li(n, )3H reactions.
Additionally, to determine the background causedby high-intensity gamma-rays, a 7Li-glass detector (depleted in 6Li) has also been installed. The scintillator of
the 7Li-glass detector was GS-30 (7Li enrichment higher
than 99.99%) manufactured by Saint Gobain with thesame size and chemical component of the 6Li-glass
scintillator. The 7Li-glass detector is set on the upstreamside of the 6Li-glass detector. The signals from the photomultipliers (HAMAMATSU:H7195) are analyzed using CAEN V1720 (12-bit 250 MHz) module with digitalpulse processing software, DPP-CI. The module records
a pulse height and a time of flight in “event-by-event”
mode.
3. Neutron total cross section measurement of 241Am
In recent years, total cross sections of 241Am and243Am were measured in ANNRI [3, 4]. As an exampleof the measurements, the neutron total cross section
measurement of 243Am are reported.
For the experiment, a 243Am sample with nominal
activities of 240 MBq was prepared. The sample wasencapsulated in Al containers with diameter of 22 mm
and thickness of 0.1 mm. Similarly, a “dummy sample”
without Am sample was prepared. The 243Am sample
and the dummy sample were set on the neutron beamline at the flight length of 24.5 m. Transmission neutrons were detected with the Li-glass detectors. The
total measuring time was about 16 hours for the 243Am
sample and about 8 hours for the dummy sample.
The TOF spectra of the 243Am sample and the dummy sample with the Li-glass detectors are shown in
Fig. 2. Dead-time correction and background subtraction were applied. The transmission ratio of the 243Am
sample was obtained.
The deduced total cross section of 243Am is shownin Fig. 3. The cross section was derived using the transmission ratio of the sample and the areal density of the243Am sample.
Using our new detectors and DAQ, total cross section of 243Am was derived in the neutron energy range
from 4 meV to 100 eV.

MLF Annual Report 2018

Neutron Science

Figure 2. TOF spectra of the 243Am sample and the dummy
sample with the Li-glass scintillation detectors [4].

Figure 3. Derived total cross section of 243Am, and uncertainties of the cross sections (total, statistical uncertainty, systematic uncertainty, uncertainty due toneutron intensity, and uncertainty due to impurity
subtraction) [4].

References[1] M. Salvatore, R. Jacqmin, “Uncertainty And Target
Accuracy Assessment for Innovative Systems using Recent Covariance Data Evaluations.” WPEC-26,
OECD NEA, (2008).
[2] H. Harada, et al., J. Korean Phys. Soc. 59, (2011) 1547.

[3] K. Terada, et. al., Journal of Nuclear Science andTechnology, (2018), https://doi.org/10.1080/00223
131.2018.1485519[4] A. Kimura, et. al., Journal of Nuclear Science andTechnology, (2018), https://doi.org/10.1080/00223
131.2019.1598508

A. Kimura and S. Nakamura
Nuclear Data and Reactor Engineering Division, Nuclear Science and Engineering Center, Japan Atomic Energy Agency

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Status of Fundamental Physics Beamline BL05 (NOP) in2018

2. Measurement of the neutron lifetime
A neutron decays into a proton, an electron, andan antineutrino. The decay lifetime is an important parameter for the unitarity of the CKM matrix and also
for the primordial big bang nucleosynthesis. However,recently reported values for the neutron lifetime deviate significantly from the systematic uncertainties. An
experiment to measure the neutron lifetime with apulsed beam is ongoing at BL05 (NOP). The lifetime ismeasured as a ratio of the electron events of the neutron decay to the 3He(n,p)3H events caused by 3He gas
precisely doped in a time-projection chamber (TPC). By
analyzing the data, we obtained our first preliminary
result of the neutron lifetime as n  896  10 (stat.) 1410(sys.) [4].

3. Development of a sub-micrometer position
sensitive neutron detector using nuclear emulsion
Nuclear emulsion, which is a kind of photographic
film, is used as a high-sensitivity position tracking detector for particle and nuclear physics. An ionizing particle passing though the emulsion makes fine grains
along its track. Observing the grains by a microscope,
the track can be reconstructed very precisely.
We applied the nuclear emulsion to neutron detection with sub-micrometer spatial resolution [5]. The
detector consists of 10B and cover layers on Si substrate.
Nuclear emulsion of 10 m thickness was coated on it(Fig. 2 Left). Neutron that makes 10B(n, )7Li reaction at
the 10B layer emits either an particle or 7Li-ion into the

Neutron lifetime [sec]1. Introduction“Neutron Optics and Physics (NOP/BL05)” at MLF
in J-PARC is a beamline for studies in the field of fundamental physics. The beamline is divided at the upstream into three branches, the so-called Polarized,
Unpolarized, and Low-Divergence branches, used indifferent experiments in a parallel way [1–2].
A neutron lifetime measurement is conducted at
the Polarized beam branch with a spin flip chopper.
Pulsed ultra-cold neutrons (UCNs) by a Doppler shifter
are available at the Unpolarized beam branch. At the
Low-Divergence beam branch, the search for an unknown intermediate force is performed by measuring
neutron scattering with rare gases. The beamline isused also for R&D of optical elements and detectors [3].

915
910
905
900
895

㻤㻚㻠㻌㼟㼑㼏㻌㻔㻠㻌σ㻕㻌㻌

890
885
880
875
1990

1995

2000

2005

2010

2015

Figure 1. The neutron lifetime measurements in the 2017
PDG [1], the storage methods are denoted as blue
squares, the proton counting is shown as closed
red circles. The J-PARC preliminary result is shown
as a red open circle [3].

Figure 2. (Left)A schematic view of the detector. (Right) Position errors of detected tracks in longitudinal
and transverse directions with the track angles (tanθ).

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emulsion layer, whose track lengths are 5.1 and 2.6 m,
respectively. Reconstruction analysis of the grains by the
track can determine the starting position of the track
where the neutron was captured by 10B. The error of thestarting position depends on the track angle to the substrate, . If we select tan() 1.9, which corresponds toacceptance efficiency of 34%, the spacial resolution to
the longitudinal direction is estimated to be 11–99 nm.
The resolution to the transverse direction was estimatedas 11 nm independently in the track angle (Fig. 2 Right).
This unprecedented spatial resolution detector canbe applied for various experiments involving neutron
quantum effects or sub-micro neutron imaging.
References[1] K. Mishima et al., “Design of neutron beamline

Neutron Sciencefor fundamental physics at J-PARC BL05,” Nucl.
Instruments Methods Phys. Res. Sect. A, vol. 600, no.
1, pp. 342–345, 2009.
[2] K. Mishima, “J-PARC Neutron fundamental physics
beamline (BL05/NOP),” Hamon Neutron Netw. news,
vol. 25, no. 2, pp.156–160, 2015.
[3] K. Mishima et al., Fundamental physics activities
with pulsed neutron at J-PARC (BL05). Proceedingsof International Conference on Neutron Optics(NOP2017) JPS Conference Proceedings, Vol. 22(2018) 11033. (arXiv:1712.06351, 2017)[4] N. Nagakura et al., PPNS2018, Grenoble, France.
[5] N. Naganawa et al., “A Cold/Ultracold Neutron
Detector using Fine-grained Nuclear Emulsion with
Spatial Resolution less than 100 nm”, European
Physical Journal C (2018) 78: 959.

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

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BL06: Commissioning Status of VIllage of Neutron
ResOnance Spin Echo Spectrometers (VIN ROSE)
1. Introduction
Neutron spin echo (NSE) is a variety of neutron
spectrometry for high-resolution inelastic and quasielastic neutron scattering methods [1]. Because the energy resolution of the energy transfer measurement is
not limited by the energy spectrum of the incoming
neutrons in the NSE technique, a moderately (10–15%
FWHM) mono-chromatic neutron beam is acceptable.
In addition, the intermediate scattering function can bedirectly derived by NSE, so that the method is suitable
for studying slow relaxation dynamics in condensed
matter, and high-intensity and high-energy-resolution
NSE spectrometers have been developed and built [2].
Since 2011, Kyoto University and The High Energy
Accelerator Research Organization (KEK) have been
jointly constructing beamline 6 (BL06), which consistsof two types of NSE spectrometers with neutron resonance spin flippers (RSFs), that is, a neutron resonancespin echo (NRSE) instrument and a modulated intensity by zero effort (MIEZE) instrument, at Materials andLife Science Experimental Facility (MLF), Japan Proton
Accelerator Research Complex (J-PARC) [3]. The spectrometers use RSFs, which can replace large magnetic
precession fields with low guide fields, therefore downsizing and adjacence of the spectrometers become
possible [4].
In this report, the status of the MIEZE and NRSE
spectrometers at BL06 in FY2018 is summarized.
2. Commissioning status at BL06 in FY2018
Time-of-flight neutron spectroscopy and MIEZE(TOF-MIEZE) is a novel approach. We have verified quantitatively fundamental characteristics of TOF-MIEZE [5].
Since the 2017B proposal round, the user program has
been partially started with the MIEZE spectrometer,
which will be described in the following section in detail.
At the NRSE spectrometer, used for high-energy
resolution, commissioning of the devices such as RSFs
and two-dimensional ellipsoidal neutron-focusing mirrors were intensively conducted. The 5Qc NiC/Ti twodimensional ellipsoidal neutron-focusing supermirrors,
where xQc means that the critical angle is x times larger,
were developed in close collaboration with the RIKEN
center for advanced photonics [6]. The optical design
includes 1250 mm semi-major axis and 65.4 mm semiminor axis with 900 mm length, as shown in Fig. 1.
84

Figure 1. Partial cross-sectional view of the ellipsoidal neutron-focusing mirror (see ref. [6]).

By using the mirrors, the characteristics of the spectrometer were evaluated quantitatively. The achieved findings will be applied to the further developments of the
NRSE spectrometer.
3. User Program
The great advantages of the MIEZE spectrometeris that relatively strong magnetic field in any direction
can be added in the sample position. This characteristic
is very appropriate for studies of slow-spin dynamics onmagnetic properties, such as the Skyrmion phase observed in magnetic substances [8]. In order to executesuch kind of investigations, a 4K GM cryostat and a very
compact magnet, which can add maximum 0.2 T at the

Figure 2. The sample stage of the MIEZE spectrometer,where a 4K GM cryostat and a 0.2 T permanent
magnet at the sample position are installed.

MLF Annual Report 2018

sample position, have been installed to the instrument.
Figure 2 shows the cryostat and the magnet at the sample stage, where the magnetic field is parallel to thebeam propagation direction, which is normally impossible for generic “Mezei type” spin echo spectrometers.
We have been able to observe 200 kHz MIEZE signals(corresponding to maximum 2 ns Fourier time) clearlywith this geometry. Five user programs in total werecarried out with the MIEZE spectrometer in FY2018 inaddition to internal studies, in which three topics wererelated to magnetism.
4. Summary
The current status of BL06 VIN ROSE in FY2018 was
briefly reported. The public use has been started partially with the MIEZE spectrometer. A 4K GM cryostat and acompact maximum 0.2 T permanent magnet are available as sample environments. At the NRSE spectrometer,
the two-dimensional ellipsoidal neutron-focusing supermirrors with 5Qc were tested, which was essential forthe development of NRSE with high-energy resolution.
Acknowledgments
We thank Dr. T. Hosobata and Dr. Y. Yamagata

Neutron Science

at RIKEN Center for Advanced Photonics for providing the substrates of the two-dimensional ellipsoidal
supermirrors.
References[1] F. Mezei ed., Neutron Spin Echo, Lecture Notes inPhysics, (Springer, Berlin) 128, (1982).
[2] D. Richter, M. Monkenbusch, A. Arbe, J. Colmenero,Adv. Polym. Sci. 174, (2005) 1–221.
[3] M. Hino, T. Oda, M. Kitaguch, N.L. Yamada, H.
Sagehashi, Y. Kawabata, H. Seto, Physics Procedia 42,(2013) 136.
[4] R. Gähler and R. Golub, J. Phys. France, 49, (1988)
1195–1202.
[5] T. Oda, M. Hino, H. Endo, N.L. Yamada, Y. Kawabata,H. Seto, JPS Conf. Proc. 22, (2018) 011010.
[6] T. Hosobata, M. Hino, H. Yoshinaga, T. Kawai, H. Endo,
Y. Yamagata, N. L. Yamada, S. Takeda, JPS Conf. Proc.
22, (2018) 011010.
[7] H. Endo, T. Oda, M. Hino, T. Hosobata, Physica B 564,
(2019) 91.
[8] S. Mühlbauer, B. Binz, F. Jonietz, C. Pfleiderer, A.
Rosch, A. Neubauer, R. Georgii, P. Böni, Science, 323,
(2009) 915.

H. Endo1,2, M. Hino3, T. Oda3, N. L. Yamada1,2, H. Seto1,2, and Y. Kawabata3
Neutron Science Division, Institute of Materials Structure Science, KEK; 2Neutron Science Section, Materials and Life Science Division,
J-PARC Center; 3Institute for Integrated Radiation and Nuclear Science, Kyoto University

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Current Status of BL08 SuperHRPD in 2018
1. Introduction
Super High-Resolution Powder Diffractometer(SuperHRPD) is a neutron powder diffractometer withsuper high resolution, which in 2008 achieved theworld’s best resolution (d/d  0.035%) among similar
diffractometers [1]. SuperHRPD is one of the day-one
instruments and has been in operation for 10 years. The
construction of the instrument has been completed
and its main task is to perform general user programs.
However, the expansion of the instrument’s capabilities
is gradually progressing to make it more useful in thedevelopment of advanced science.
2. A breakdown of the total beam time in FY2018
In FY2018, SuperHRPD performed 911 measurements, and all 12 proposed general user programs
could be carried out. SuperHRPD has several instruments for sample environment and the breakdown ofusage in FY2018 is shown in Fig. 1. About half of the total
measurement time was occupied by low-temperatureexperiments using a cryostat, 20% was room temperature measurement by auto sample changer, 10% was
high-temperature measurement by vanadium furnace,
and the remaining 17% as commissioning the 14-Tesla
magnet. Two of the cryostats we own are older models that have been in use for 20 years since the KENS
era, and it is hoped that they will be upgraded to new

Figure 1. Operating ratio of the sample environment in total measurement time in FY2018. The total measurement time in 2018 was about 4000 hours, and
911 measurement data could be obtained. Of thegraph legends, 1K, 4K, New4K, and TL are lowtemperature devices, and TL is a Top-Loading type.
A.S.C. indicates an Auto Sample Changer used forroom temperature measurement.

86

equipment with improved performance. Considering
the environment for low-temperature experiments, theintroduction of more advanced cryo-furnace that cancontinuously measure from low to high temperatures
is in progress.
3. Official start of a Fast Track Proposal
The three beamlines, SuperHRPD, NOVA and
PLANET, have officially started a Fast Track Proposal(mail-in program). In FTP, the user sends their samples tothe MLF, and the MLF staff performs the experiment onbehalf of the user and sends them the data. Currently,
there is a limit of 24 hours per one proposal, but withinthat time, room temperature measurement using an
auto sample changer and low temperature measurement using a cryostat can be performed. SuperHRPD
has conducted this proposal on a trial basis in advanceand has completed seven proposals by the end of
FY2018. FTP is useful for beamline groups with limited
manpower like ours, and is a useful system for effective
beam usage, like taking advantage of beam time that isvacant on the weekends and time adjustments to avoid
user change at midnight.
4. Installation and commissioning of several devices
An electric 4-quadrant slit system (Fig. 2) was installed at incident side of the sample vacuum chamberof SuperHRPD. Until now, a simple manual incident
beam slit using a sintered B4C plate was used, but
this motorization is expected to shorten the time of

Figure 2. (Left) 4-quadrant slit system installed in SuperHRPD.
A slim shape with a width of 10 cm was realized bydevising the arrangement of the stepping motor.
(Right) Slit control GUI created using LabVIEW.

MLF Annual Report 2018changing the slit and improve the reproducibility of theslit size. On the incident side of the sample chamber,there was only a small space between the left and rightbackscattering banks, so a narrow-slit system was required. By efficiently arranging four stepping motors,
we were able to complete a slit system with a width of
only 10 cm. In addition, we built a slit control systemusing LabVIEW and completed a visually operable program with an emphasis on GUI.
A commissioning of 1K cryostat (Fig. 3) owned by
the SuperHRPD group was carried out in the second
half of FY2018. Since this cryostat was introduced at thetime of the Great East Japan Earthquake, its commissioning was delayed because various restoration tasks
had been prioritized. First, we performed backgroundmeasurement and correction data measurement using
a neutron beam without cooling. By adjusting the incident beam slit, we were able to suppress unnecessaryreflections and obtain good background data. After
that, we conducted a cooling test of the 1K cryostat
system at the off-beam line. Compressors and otherdevices showed healthy operation were not affectedby the earthquake disaster, but we found out that theessential 3He gas line needle valve had a problem anddid not reach the minimum temperature. Maintenance

Neutron Science

Figure 3. The 1K cryostat system during commissioning. A
problem was found with the needle valve in the3
He line, and repair is scheduled for FY2019.

performed by the manufacturer is scheduled for 2019,
and after that, the normal operation is expected toresume.
References[1] S. Torii et. al., J. Phys. Soc. Jpn. SB020 SB020-1-4(2011).
[2] http://j-parc.jp/researcher/MatLife/en/applying/
FTP_v01.html

S. Torii1,2, M. Hagihala1,2, 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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Current Status of SPICA in 2018
1. Introduction
In the charge/discharge reaction of a real batteries, neutron diffraction with wavelengths of atomic
distances is used to analyze the change of atomic arrangement including mobile ions at the atomic level.
This method can provide the positional information oflight elements with relatively high accuracy. The structural analysis of actual battery electrodes by neutron
diffraction is an indispensable technique for elucidating degradation behavior. We are establishing the operando techniques of real batteries by non-destructive
in situ observation, and proceeding with innovative
battery research by relating electrode degradation withstructural variation.
2. A new data processing computer system
One of features of MLF experiments is a data acquisition system called an event method where eachneutron that enters into every detector pixels can berecorded as an event. After the experiment, the experimental data can be reproduced in various histograms
depending on the specific objectives. However, since

Figure 1. A new SPICA data processing computer system.

the event method generates a large amount of event
data at the same time, the data processing is a big
problem. The SPICA data processing computer system
supports the data acquisition and data reduction. Over
7 years have passed since the old system started, andits service life has been exceeded, so a new system wasintroduced. The new system is designed to be fasterwith reduced cost while maintaining the performance.
Furthermore, the virtual technology was introduced toreduce the number of data processing computers byhalf. The number of computers required for has been
halved. Figure 1 shows the computer system. Data reduction performance such as time-dependent histogramming has improved as shown in Table 1, which isbeneficial for operando experiments.
3. Bragg edge imaging
The Neutron Bragg-edge Imaging (NBI) has been
expected to visualize a wide area of a real battery atonce. There is no such technology for imaging the density of electrolyte solution which can be used for innovative batteries. In order to develop the NBI technology
for visualizing electrolyte concentration in LIB, experiments were conducted using samples in which electrolytes were dissolved at different concentrations in theelectrolyte solution. The specimens were prepared bydissolving 0.0 M, 0.5 M, 1.0 M, 2.0 M, and 3.0 M of electrolyte LiPF6 in an electrolyte solution (mixed solutionof ethylene carbonate, dimethyl carbonate, and ethyl
methyl carbonate) placed in an aluminum container
with a thickness of 5 mm. At SPICA, these specimens
were placed in the neutron beam, and the neutrons
that passed through the specimen were detected by
an NBI two-dimensional neutron detector installed
downstream of the specimen. Figure 2 shows the twodimensional neutron distribution in various electrolyte
concentrations. A bright area of 65 mm  18 mm is the
sample area containing the electrolyte of 0.0 M to 3.0 M
while the outside is shielded against neutrons. For theregion inside the red dashed line in Fig. 2, the neutron
wavelength-dependent transmission was obtained by

Table 1. Data reduction performance.

88

High speed processing (s)Serial processing (s)Time-dependent processing (s)Old system

1184

2416

2282

New system

635

1247

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MLF Annual Report 2018

dividing the data of 0.0 M–3.0 M electrolytes by that of
the aluminum empty container. The obtained transmission is shown in Fig. 3. The longer the neutron wavelength, the lower the transmission, which is consistent
with the neutron absorption by hydrogen and 6Li.
The transmission spectra slightly vary dependingon the electrolyte concentration. In order to extract theslight variation in area densities of the electrolyte solutions, transmission data were fitted with a function

Neutron Scienceof the sum of the calculated LiPF6 transmission andexperimental transmission of 0.0 M. Here, this function includes the area densities of the electrolyte andthe electrolyte solution as fit parameters. The results offitting are shown in the solid line in Fig. 3. The broken
line is a fit with a function that does not contain LiPF6,
indicating that the solid line is in better agreement withthe experimental spectrum, especially for samples withhigher electrolyte concentrations.

Figure 2. Two-dimensional neutron distribution in various electrolyte concentrations.

Figure 3. Transmission spectra in various electrolyte concentrations.

T. Kamiyama1,2, M. Yonemura1,2, S. Torii1,2, T. Saito1,2, and K. Kino3
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3ResearchInstitute for Measurement and Analytical Instrumentation, AIST

1

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BL10: NOBORU
1. Introduction
In FY2018, twelve general-use proposals and two
project-use proposals, in addition to the postponed two
proposals from FY2017B, were carried out at NOBORU.
The user program was not disrupted by any technicalproblems with the instruments.
This year, we made an attenuation chopper which
can selectively suppress the spectral peak of the thermal neutrons and helps to relax the counting limit of
the imaging detectors [1]. Its basic design and performance test are described in Section 2.
2. Design and performance of the attenuation chopper
When performing Bragg-edge imaging experiments, the beam collimation ratio (L/D) is often set tovery large values, for example L/D  2000, not to prevent
image blurring but rather to match the counting limit of
the 2D detector. In practice, L/D values and field of vieware determined by checking the direct beam spectrum
to prevent event loss due to pile-up at a peak flux ofabout 2.3 Å. As a result, the detector is easily operated
in the cold neutron region. Therefore, it is desirable toattenuate only the thermal peak region and make thespectrum flatter.
The specific requirements are as follows: a) attenuating thermal neutron by 1/2 ~ 1/3, b) low background ofneutrons and gamma-rays, c) low electric noise, and d)table-top size and weight. To fulfill these requirements,
we designed the attenuation chopper shown in Fig. 1.
The chopper blade weighs about 0.4 kg and can be rotated by a 24 V DC motor, which produces negligible
electrical noise inside the experiment room. The TEMPAX
Float® scatters neutrons little, and generates low-energy
gamma-rays compared with the sample’s ones.
The design validation was performed by using
a monitor counter under weak beam conditions. No
event loss was confirmed for the spectrum obtainedby open-stop position (blue dots in Fig. 2). Next, theattenuation chopper was kept in a close-stop position
and the obtained neutron spectra (left axis) and its exponential decay ratio (right axis) were plotted by green
dots. Finally, we obtained a red colored neutron spectrum. Its counting ratio was as expected by operating
the attenuation chopper at 25 Hz and is shown in Fig. 2.
An example of Bragg-edge transmission spectrausing the attenuation chopper is shown in Fig. 3. The
chopper phase needs to be adjusted to a slightly shorter wavelength, but the transmission data was obtained
as expected. No fake humps or unexpected backgroundwere found in the whole spectra.

Figure 1. Picture of the attenuation chopper with the outer
cover removed. The blade is in open-stop position.

Figure 2. Measured neutron spectra and their ratios at three
chopper conditions. Blue: open-stop position, green:close-stop position, and red: operating at 25 Hz.

Figure 3. Incident neutron, transmitted neutron, and theirtransmission spectra of a ferrite steel sample obtained by a single pixel of nGEM detector.

Reference[1] J. D. Parker et al., JPS Conf. Proc. 22, 011022 (2018).

K. Oikawa
Neutron Science Section, Materials and Life Science Division, J-PARC Center90

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Neutron Science

BL11: Development of Neutron Imaging Techniqueunder High-Pressure Condition
1. Introduction
Radiography is an effective technique to see the internal structure of materials. Compared to X-ray radiography, neutron radiography has an advantage in observing
light elements and isotopes via unique interaction ofneutrons with them. These two characteristics enable observation of water distribution in minerals in a high-pressure cell as well as determination of diffusion constantunder high-pressure and high-temperature condition.
By conducting neutron radiography for samples at highpressures and high temperatures relevant to Earth’s mantle condition, we can understand the role of water on materials cycle in the Earth’s interior. This year we have tried
to establish neutron radiography under high-pressureand high-temperature condition at PLANET [1].
2. Experimental setup
One of the problems in neutron radiography underhigh-pressure condition is the degradation in spatial
resolution of the obtained images due to aberration.
It is caused by a finite sample-camera distance L (i.e,neutron camera cannot be placed just behind sample
because of interference with a high-pressure press) anda large divergence of the incident neutron beam. So far,
we tried high-pressure neutron radiography by coupling a bulky neutron camera (Toshiba, Neutron Color
I.I.TM) with the six-axis press ATSUHIME [2]. The achieved
resolution was limited to 400 m because the large
body of the camera prevented us from placing it close
to the sample (L  146 mm).
To overcome this problem, we newly employed acompact neutron camera (ADVACAM, MiniPix ver.1.0)
with size similar to that of a USB stick. This makes it possible to reduce the sample-camera distance down to L
 88 mm (Fig. 1), which has significantly improved thespatial resolution as shown below.
3. Optimization of the parameter of beam optics
Prior to the radiography experiments at high pressures, we evaluated the effects of beam optics on the
resolution without using a press. For the evaluation,
we took images of a pattern lithographed with Gd on
silica glass as functions of the sample-camera distance(L) and the width of 2nd beam narrower (S2), which was
located at the exit of the beam transfer tube. The S2
defines the length-aperture (L/D) ratio that strongly

affects the resolution. By reducing the S2 value from
10 mm to 2 mm, the L/D ratio can be changed from 200
to 1000 continuously.
Figure 2 shows the S2 and L dependence on the spatial resolution. Here, the resolution was estimated fromthe width of the fringe of the Gd pattern in the obtained
images. The resolution was found to be 100 m regardless of the S2 value when the camera was placed just behind the sample (i.e. L  0 mm). The resolution became
worse as the L increased, and the degree of the worsening became more prominent for the larger S2 value. This,
however, does not necessarily mean that the smaller S2 ispreferable because it also reduces the flux of the incident
beam, which decreases the contrast of images. After several tests, we finally determined the optimum value forS2 as 6 mm. In this condition, we can obtain one image
with the spatial resolution of 200 m and the contrast
resolution of 10% by a single shot with 10 min exposure.

Figure 1. Neutron camera mounted on the six-axis press.

Figure 2. S2 and L dependence on the spatial resolution.

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4. In-situ observation of H-D interdiffusion in brucite
at 5 GPa and 1100 K
As a test of the neutron radiography under highpressure and temperature condition, we observed theinterdiffusion of hydrogen and deuterium atoms in
brucite (Mg(OH)2) at 5 GPa and 1100 K. This substanceis of geophysical importance because it is a simplified
form of hydrous minerals, which play an important rolein transporting water into the Earth’s interior. The highpressure cell used in this study is shown in Fig. 3. The
pellets made of Mg(OH)2 and Mg(OD)2 powder werestacked and packed in a Pt capsule to seal the hydrogen. This was placed in a graphite tube heater and encased in a ZrO2 pressure transmitting medium, together
with a MgO electric insulator. This cell was compressedto 5 GPa and then heated to 1100 K for 27 hours. The
neutron images were taken for 10 min per each at selected elapsed times. Figure 4 shows the obtained radiographs. The images were taken through the gap
between the WC anvils opaque to neutrons. Thus, thefield of view was limited to 1.4 mm in width. In spiteof this limitation, a clear contrast originating from difference in the transmittance between H and D atoms
was observed. With time, the boundary between them
became obscure, suggesting that the inter-diffusionof H/D occurred at the interface. Figure 5 shows the

diffusion profiles obtained by integrating the intensity
in the center region along the vertical direction. By analyzing the profiles with the Boltzmann–Matano method,
we obtained interdiffusion constant of 11.0  0.2 m2/s,
which was consistent with the value reported so far [3].

Figure 4. Time evolution of the radiograph.

Figure 5. Diffusion profiles obtained by integrating intensity
in the center region along the vertical direction.

Figure 3. The high-pressure cell used in the experiment.
The unit is mm.

References[1] T. Hattori, et al., Nucl. Instrum. Methods. Phys. Res.,
Sect. A780 55 (2015).
[2] A. Sano-Furukawa et al., Rev. Sci. Instrum. 85 113905(2014).
[3] Guo et al., Amer. Mineral, 98 1919 (2013).

H. Arima1, T. Hattori2, A. Sano-Furukawa2, S. Machida1, J. Abe1, and K. Funakoshi1
Neutron Science and Technology Center, CROSS; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center

1

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Neutron Science

High Resolution Chopper Spectrometer HRC
1. Introduction
The High Resolution Chopper Spectrometer (HRC)
is being operated at BL12 in MLF to study dynamics incondensed matter, especially in wide range of correlated electron systems. The HRC delivers high-resolution
and relatively high-energy neutrons, and we proposed
three types of inelastic neutron scattering (INS) experiments on the HRC: high-resolution experiments
in a conventional energy momentum space, neutron
Brillouin scattering (NBS), and sub-eV neutron spectroscopy. In the first phase of the HRC project in the period
between FY2008 and FY2013, we constructed the HRC
and confirmed that it performed as expected. Based on
the achievement in the first phase, we planned to improve further the performance of the HRC in the second
phase in the period between FY2009 and FY2018. The
improvements focused on two subjects: a realization ofpractical use of NBS experiments and a demonstrationof INS under external fields. The results from the instrumentations for NBS and INS under external fields are
the detections of Weyl fermions in metallic ferromagnet
SrRuO3 and novel excitations near quantum criticality
in geometrically frustrated antiferromagnet CsFeCl3,
respectively.
2. Instrumentation
NBS is INS near the forward direction, and therefore, the performance of devices on the beamline,
which are the low-angle detectors, the collimator system, and the Fermi chopper, is important [1]. In the
low-angle detector bank at the secondary flight pathof L2  5.2 m, position sensitive detectors (PSDs) werealigned in a double-layered configuration to increase
the counting rate. The distortion of the slit package of
the Fermi chopper was improved. The geometry of theslit package of the high-resolution Fermi chopper was
optimized to obtain a large intensity while keeping highresolutions. The collimator system, which is installed at
the upper stream of the sample to reduce the background noise at low scattering angles, was improved.
After these improvements, an intensity gain of a factorof 3.5 was achieved for the incident neutron energy ofEi  100 meV with the energy resolution of E  2 meV.
Moreover, a resolution of nearly 1% was achieved withan acceptable intensity for E  1.4 meV at Ei  100 meV(E/Ei  1.4%).
A superconducting magnet was installed. Althoughan operation at 10 T was confirmed on the HRC, avacuum leak occurred. The manufacturer evaluated the
maximum magnetic field to be 5 T under the environment on the HRC. We will plan to perform experiments
using the magnet below 5 T in the next phase of the
HRC project. Realizing INS experiments under external
fields is important issue on the HRC. We tried to perform INS experiments under high pressures insteadof magnetic fields. A standard sample can, containing
a cylindrical pressure cell with a sample crystal up to
1.5 GPa, was successfully cooled with a refrigerator.
We have constructed computing system and software environment to control accessories and to handle
neutron signals from PSDs for the HRC. In the softwareenvironment, comprehensive control program YUI andvisualization program HANA play central roles. During
this period, we completed successfully YUI and HANA,and now we can conduct experiments confidently [2].
Other instrumentations are briefly described. In thefirst phase, we installed 128 pieces of PSDs with dimensions of 2.8 m long and 19 mm diameter and 1.8 MPa
of 3He gas pressure to cover the scattering angles  
3° – 42° at L2  4 m. PSDs at L2  4 m were increased to
256 pieces, which are mounted at   3° – 62.5° and  −14° – −29.6°. We have a variety of sample environments: a GM type refrigerator (T  3 K), a 3He sorption
pumping type refrigerator (T  0.6 K), a 3He circulation
type refrigerator (T  0.3 K). In the 3He refrigerators,
background noise is generated at their outer vacuum
chambers. By installing an oscillating radial collimator, the background noise has been reduced. Frequent
maintenance works were performed for vacuum systems, choppers, refrigerators, and computing systems.
3. Scientific results
An anomalous Hall effect (AHE) is a Hall effect in aferromagnet, where the Hall resistivity is proportional
to the spontaneous magnetization M. However, theAHE in SrRuO3 cannot be described by such a simple relation. SrRuO3 exhibits a band structure including bandcrossing. The band crossing (Weyl fermion) produces
the Berry phase, the Berry curvature takes the form ofa magnetic monopole in the momentum space, andthen, the fictitious magnetic field is an origin of the
AHE. It is known that the Hall conductivity xy in SrRuO3
can be well described by this picture. For SrRuO3, alarge single crystal necessary for INS has not been synthesized. Therefore, NBS on the HRC using a powder
sample is the only way to observe spin waves in SrRuO3.
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The observed spin wave dispersion relation can be wellfitted to E(Q)  DQ2Eg, and the spin wave gap Eg shows
nonmonotonous temperature (T) dependence (Fig. 1).
We found that the observed Eg is well explained by atheoretical form: Eg(T)  aM(T)/[1bxy(T)/M(T)], where
Eg can be described by the Berry curvature through xy.
We showed that the Berry curvature, that is the fictitious
magnetic field produced by the Berry phase, is an observable of INS [3]. Correlated electronic systems havethe internal degrees of freedom such as spin, charge,
orbital, lattice, etc. The fluctuations of these degrees
can be observed as spin waves, orbital waves, phononsetc. by means of INS, which are influenced by the quantal phase of electronic wavefunctions.
In a spontaneously symmetry-broken state near
the quantum critical point (QCP), the phase and amplitude fluctuations of the order parameter are observed
as the gapless Nambu-Goldstone and the gapped
Higgs modes, respectively. We observed a hybridizationof the phase and amplitude fluctuations near QCP in afrustrated magnet CsFeCl3. A triangular-lattice antiferromagnet CsFeCl3 shows a quantum disordered stateat ambient pressure, and an ordered state with a noncolinear spin structure above the critical pressure (PC 0.9 GPa). We performed INS experiments under several pressures using HRC and the triple axis spectrometer CTAX at ORNL. Below PC, a gapped spectrum wasobserved. On the other hand, we observed a gapless
spectrum as well as characteristic excitations at 0.5 –0.8 meV and 0.8 – 1.3 meV above PC (Fig. 2). In order todiscuss the observed spectra, the one-magnon crosssection was calculated based on the extended spinwave theory (ESW). One-magnon processes for the
hybridization between the phase and amplitude fluctuations can only exist in a noncollinear state and thetwo characteristic excitation modes show level repulsion. The observed spectra agree well with this calculation. However, the two modes simply cross without the
hybridization, and this calculation does not reproduce
the observation. The hybridization plays an importantrole in magnon dynamics in noncollinear magnets near
QCP. The INS measurements in CsFeCl3 revealed this by
the fine tuning of pressure through QCP [4].

Figure 1. Spin wave gap Eg(T) (a) and anomalous Hall conductivity σxy(T) (b) in SrRuO3 as a function of T/TC with TC =165 K. The solid line in (a) is a fitted curve described in
the text. (Reproduction from Ref. [3].)Figure 2. INS spectra from CsFeCl3 obtained at HRC under (A)0.0 GPa at 6 K and (B) 1.4 GPa at 0.9 K. The marks are theexcitation peak positions obtained at CTAX. The solid
yellow curves are calculated by ESW. (Reproduction
from Ref. [4].)Moreover, we have successfully investigated spin
dynamics in correlated electron systems with the conventional method of INS [5–9].
References[1] S, Itoh, et. al., Physica B, 568 76 (2019).
[2] D. Kawana, et al., J. Phys.: Conf. Series, 1021 012014(2018).
[3] S. Itoh et al., Nat. Commun., 7 11788 (2016).
[4] S. Hayashida et al., Sci. Adv., 5 eaaw5639 (2019).
[5] S. Hayashida et al., Phys. Rev. B 92, 054402 (2015).
[6] Y. Ikeda et al., J. Phys. Soc. Jpn. 85, 023701 (2016).
[7] S. Ibuka et al., Phys. Rev. B 95, 224406 (2017).
[8] T. Haku et al., J. Phys. Conf. Series 828, 012018(2017).
[9] D. Ueta et al., Physica B 536, 21 (2018).

S. Itoh1,2, T. Masuda1,3, T. Yokoo1,2, S. Asai3, H. Saito1,2, D. Kawana3, R. Sugiura3, T. Asami3, and Y. Ihata4
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 Center

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Neutron Science

BL14 AMATERAS
1. Introduction
FY2018 was the tenth year of operation of
AMATERAS [1, 2], a cold-neutron disk-chopper spectrometer. We continued the user program out-reachactivities. As a part of our upgrade program, we havecarried out detector and detector bank related equipment enhancement. In this FY, we did not encounterany serious mechanical problems with the equipmentof AMATERAS.
2. User program, international activities and out-comes
The number of short-term general proposals submitted for the 2018A and 2018B periods was 31 (accepted: 14, reserved: 16, not approved: 1) and 24 (accepted:
13, reserved: 10, not approved: 1), respectively. We also
had two long-term general proposals (accepted: 1, notapproved: 1), three urgent proposals and three JAEA
project proposals. The majority of the proposals dealt
with studies on magnetism and strongly correlated
systems, especially subjects related to quantum spin
systems. As a result, in FY2018, 29 short-term general
proposals, one long-term general proposal, three urgent proposals and three JAEA project proposals werecarried out on AMATERAS.
In 2018, 14 refereed papers covering the woks at
AMATERAS were published. The research topics included thermo-electric materials, novel superconductors,
quantum spin liquids, 4f electron systems and othermagnetisms. Furthermore, one press releases was issued, which covered the study on quantum paramagnet near spin-state transition in Co oxides done bya research group headed by Dr. Keisuke Tomiyasu of
Tohoku University.
3. Instrumental activities
When we installed 10 position sensitive detectors(PSDs) in FY2017, six of them were installed to every
other position in the high-angle side. This fiscal year,
during the summer shutdown period, we additionallyinstalled more PSDs to fill up the blankspots. As the result, the horizontal angle region up to 118° was covered(Fig. 1). This could be effective for various experiments,
such as observations of phonon spectra and molecular

dynamics. Furthermore, we added more vanes to thenegative scattering angle side in the vacuum scatteringchamber, though PSDs have not yet been installed tothis side.
We also started to prepare the replacement ofcomponents of the main vacuum pump of the scattering chamber. Some of components have already beendelivered. This upgrade will be completed in several
years.

Figure 1. Detector banks at high-angle region before and after installing PSDs. Cadmium plates are stuck on thesurface of the PSDs for calibration.

References[1] 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).
[2] K. Nakajima, RADIOISOTOPES 66, 101 (2017).

K. Nakajima1, S. Ohira-Kawamura1, M. Kofu1, T. Kikuchi1,2, Y. Inamura1, and D. Wakai3
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Chemical Analysis Center, Research & Development HQ,
Sumitomo Rubber Industries, Ltd.; 3Nippon Advanced Technology Co., Ltd.

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Upgrading TAIKAN
1. Introduction
The small and wide angle neutron scattering instrument TAIKAN (BL15) has been developed and upgradedat J-PARC to analyze precisely and efficiently the microstructures or hierarchical structures of substances invarious scientific fields with a 1-MW spallation neutron
source [1]. In FY2018, it was upgraded further to perform efficient low-q measurement and high precision
gas/vapor adsorption measurements.

measurement of porous materials, etc. (Fig. 2). The inside dimensions of the cell are 19 mm in diameter and1 – 2 mm in depth. The sample volume is about 0.3 –0.6 ml. The instrument has been used to measure specific surface area/pore size distribution, vapor adsorption
and chemisorption of a sample. The adsorption gases/
vapors to be measured are N2, Ar, H2O, D2O, etc., and themeasurement range of the pore size distribution is 0.35
– 500 nm in diameter.

2. Upgrading for low-q measurement
The detector system of TAIKAN is composed of 5detector banks: small-, middle-, high-, ultra-small-angle, and backward detector banks. On the small-angle
detector bank, 144 3He PSD tubes were additionally installed. The measurement efficiency of the small-angle
detector bank increased by about 19%. The number of
3He tubes then increased to 912, 592, 200, and 40 for
the small-, middle-, high-angle, and backward detector banks, respectively. The installation ratios of the3
He tubes became 100, 82, 36, and 50% or the small-,middle-, high-angle, and backward detector banks, respectively. Figure 1 shows a photo of the small-angle
detector bank after installing the 3He tubes.
Figure 2. High precision gas/vapor absorption measurement
instrument installed on a sample stage of TAIKAN.

Figure 1. Small-angle detector bank.

3. Upgrading for high precision gas/vapor adsorption
measurements
A high precision gas/vapor adsorption measurement instrument BELSORP-max (MicrotracBEL
Corp.) with a quartz cell was introduced for the SANS

4. Future prospects
The improvement of the measurement efficiency
by the installation of small-angle detectors and the increase of the beam intensity makes precise measurement in a low-q range easier. In the future, TAIKAN is
expected to contribute to the research of microstructures or hierarchical structures by precise measurement
not only in a low-q range but also in a wide-q range.

Reference[1] 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).

J. Suzuki1, S. Takata2, K. Ohishi1, H. Iwase1, Y. Kawamura1, K. Hiroi2, T. Morikawa1, and M. Sahara1
Neutron Science and Technology Center, CROSS; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center

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Neutron Science

Installation of Focusing Mirror for Neutron Reflectometry
at BL16 SOFIA
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 ResearchComplex (J-PARC) [1, 2]. Due to the high-flux beam of
J-PARC, less than one hour is needed for taking a fullQ-range data and only a few seconds for a limited
Q-range data in the case of a sample with 3 inches(76 mm) in diameter; even though the beam power isstill one-third of the planned value, 1 MW. However,
several hours are still needed for a small sample such as
10 mm  10 mm, which is a typical size of a sample for
X-ray reflectometry.
For further upgrade of the SOFIA reflectometer, wehave developed an elliptical focusing mirror to illuminate a 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 the mirror has an advantage on the beam flux
especially for small samples. The planned specifications of the focusing mirror and detector are a beam
size of 0.1 mm at a sample position with divergence of
2.5 mrad.
So far, we developed a prototype focusing supermirror capable of focusing neutrons with a width of
0.34 mm [3], and modified mirror with 0.17 mm in full
width at half maximum (FWHM) [4]. These mirrors work
well as focusing devices, however, the focusing size isinsufficient for our demand. Last year, we reported thedevelopment of a focusing mirror having a potential
to focus neutrons at a smaller spot size. This year, we
report the performance of the mirror evaluated withneutrons.
2. Manufacture
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 to createa smooth surface of less than 1 nm in root mean square(RMS) roughness. The super mirror with the m-value of
3 was deposited on the substrate using an ion beam
sputtering instrument at the institute for integrated radiation and Nuclear science, Kyoto University [5]. Since
the mirror size, 550 mm in length and 60 mm in width,
was too large to coat the super mirror, the mirror was
divided into two pieces and assembled into one unit
after the processes above were completed. The details
were reported in the literature [6].
3. Results
First, we summarize the results reported last year.
The surface roughness of the mirror substrate, which
is sensitive to the reflectivity of neutrons was only
0.108 nm  0.009 nm (standard deviation), that is, theroughness was better than the commercially available
Si substrates. The super-mirror coating deposited on
the substrates was very homogeneous and equivalent
to a good super-mirror guide: the critical momentum
transfer was 0.628 nm1  0.007 nm1 (standard deviation) and the reflectivity there was 86.2%  2.5% (standard deviation).
According to the surface shape of one mirror segment measured by a laser interferometer, the frequency
distribution of the slope error followed Gaussian shapewith the FWHM of 24 rad. As the distance between the
mirror and the focal point, that is, the sample position, is
designed to be 2150 mm, the minimum beam size is expected to be 50 m. However, we faced a problem withthe assembly of the two segments last year: the focal
images of the segments were not coincident at the focal
point because of the misalignment of the relative tilt.
To overcome this problem, we changed the method for fixing the mirror segments. So far, we fixed themirror segment gently with kinematic couplings. This
enabled us to minimize the stress and deformation,
but was not stable enough with respect to the vibration during transportation. Hence, we adopted direct
fixing on the flange surrounding the mirror as shown in
Fig. 1. The height of the flange at the fixing position was
precisely adjusted by a spacer, of which the length wasmachined by an ultraprecision lathe with a positioning
resolution of 10 nm.
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The new mirror has been installed at the SOFIA
reflectometer, and the focusing performance was
evaluated. Owing to the high precision of the focusing mirror shape, neutrons diverged from the slit sizeof 0.05 mm were successfully converged at the sample
position with the FWHM of 0.13 mm by the mirror. As
the slit size is adjustable using pulse motors, the beam
size at the sample position can be controlled depending on the size of the sample and incident angle to thesample plane by changing the aperture. Figure 2 shows
the beam profiles for illuminating the samples having
different sizes with the incident angle of 1.8 degrees.
Remarkably, the integral of the profiles with the focusing optics was approximately two times larger than thatwith the conventional double slit optics. This indicatesthat the exposure time for the measurement can beshortened by half by using the focusing optics for thesame data statistics.

Figure 1. Schematic illustration of the focusing mirror assembly with the direct fixing method. Each mirror is tightly fixed at ten
points on the flange with screws, and the height of the spacer is precisely machined to minimize the stress and deformation of the mirror segment.

Figure 2. Beam intensity profiles for different illumination areas at the sample position with the conventional double slit optics andfocusing optics with the mirror. The total intensity with the focusing optics is approximately twice stronger than that withthe double slits, that is, the exposure time can be shorten by half with the focusing optics for the same data statistics.

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4. Conclusion
Here, we reported the improvement of the focusing mirror developed for the neutron reflectometer
SOFIA. The latest mirror we developed can converge
neutrons on the sample position with a minimum
FWHM of 0.13 mm. The beam intensity at the sample
position with the focusing optics was approximately
twice stronger than that with the conventional double
slit optics for the same beam size, that is, the exposure
time could be shortened by half with the focusing mirror. This mirror has already been installed at the SOFIA
and used for the experiments with small samples.

Neutron Science

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] S. Takeda et. al., Opt. Express, 24, (2016) 12478–12488.
[4] T. Hosobata et. al., Opt. Express, 25, (2017)
20012–20024.
[5] M. Hino et. al., Nucl. Instr. and Meth. A, 797 (2015)
265.
[6] T. Hosobata et. al., Opt. Express, 27, (2019)26807–26820.

N. L. Yamada1,2, T. Hosobata3, M. Hino4, K. Hori2,5, F. Nemoto1,2,#, T. Kawai3, and Y. Yamagata3
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3RIKEN Center
for Advanced Photonics; 4Institute for Integrated Radiation and Nuclear Science, Kyoto University; 5Sumitomo Rubber Industory#Present aﬃliation: National Defense Academy

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BL17: Current Status of Polarized Neutron Reflectometer,
SHARAKU
1. Introduction
Neutron reflectometry (NR) is a powerful techniqueto analyze the nanostructures of the surface and interface of thin films non-destructively. In the polarized
neutron reflectometer, SHARAKU, installed at BL17 in the
MLF, not only the depth profile of the chemical composition but also the magnetic structure can be analyzed. The
large sample stage with high load capacity allows the useof various sample environment (SE) equipment, whichenables the NR measurements in various conditions,such as high magnetic field, cryogenic temperature,humidity environment and UV/visible irradiation [1–5].
In this report, we describe the status of the SE devices newly available in the NR experiments at SHARAKU.
2. Humidity Control System
The interaction between water vapor and materials
has attracted attention in industrial research and development. For example, the structure analysis of the material
in an accelerated aging test under conditions of hightemperature and humidity is necessary for the development of the performance and the quality assurance. The
NR measurement in a wide range of temperature andhumidity conditions is a key to the further improvementof the properties and functions of thin film materials suchas adhesives and polyelectrolyte membranes in fuel cells.
In order to accelerate the NR studies in this field, we
have introduced a SE system that can measure the neutron reflectivity in the controlled environment of temperature and humidity [6]. The photographs of the system
are shown in Fig. 1. This system consists of a humidity
generator (HUMICURUSE, Daiichi-kagaku Co. Ltd.) anda custom-made measurement chamber. The humidity
generator produces water vapor at the desired humidity
and temperature condition by combining dry air withsaturated aqueous vapor by two mass flow controllers.
The measurement chamber is made of stainless steel
with a cavity of 85 mm diameter and 100 mm long and iscovered with a heat insulator to introduce the temperature- and humidity-controlled gas without condensation.
The sample is placed in the center of the cavity and water
vapor flows in and out through the cavity. The incident
and reflected neutron beams pass through the Al windows installed on the both sides of the chamber. Thissetting allows the NR measurement in a humidity range
from 0 to 85% RH and a temperature range from 5 to 85°C.
100

Using this system, the structure of the polymer film
under a controlled temperature and humidity environment was measured. Figure 2 shows the neutron reflectivity profiles for a thin film of poly (vinyl alcohol) (PVA)in vapor of heavy water at various humidity values [7].
From the analysis of the NR profile, the PVA film in thedry state (at 0% RH) showed a thickness of 46 nm andscattering length density (SLD) of 0.77. At high humidity, the critical q of the total reflection increased and thegap of the Kiessig fringe decreased. This indicates that
the SLD of the film increased by the absorption of D2O
from the vapor phase and that the PVA film was swollen.

Figure 1. Photographs of the humidity-control system: sample chamber (left) and humidity generator (right).

Figure 2. Neutron reflectivity profiles of a PVA film under humidity conditions of 0, 30, 60, and 85% RH at 60°C.

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3. High-field magnets for PNR
In SHARAKU, polarized neutron reflectivity (PNR)
experiments in various magnetic fields are realized using certain kinds of magnets in the MLF. The 1 T electromagnet with a vertical magnetic field is prepared forthe usual use. For the experiments in a magnetic field
higher than 1 T, high-field magnets in the MLF can beused in SHARAKU.
The 7 T superconducting magnet is one of the highfield magnets available as common SE equipment in
MLF. The magnetic field is in the vertical direction and

Neutron Science

the sample is introduced from the top of the magnet
using a sample stick. We carried out a commissioningof this magnet to provide it for user experiments in
SHARAKU. Figure 3 shows the degree of polarization
in a system using the magnet as a result of commissioning. The flipping ratio (I/I) is more than 40 in the
wavelength range of 2.4–8.0 Å, indicating that the PNR
measurement with a high polarization contrast can be
conducted in SHARAKU. The 7-T magnet is open for user
experiments as well as the 1-T and 4-T magnets.

Figure 3. TOF spectra of polarized neutrons through an analyzer (a) and the flipping ratio in a magnetic field of
6.5 T. The red and blue dots in the panel (a) indicate the polarized neutron intensities at analyzer configurations for parallel and anti-parallel spin directions for the incident neutron, respectively.

References[1] S. Itoh, M. Nakaji, Y. Uchida, M. Kitaguchi and H. M.
Shimizu, Nuclear Inst. Meth. Phys. Res., A908, 78–81(2018).
[2] V. Ukleev, S. Suturin, T. Nakajima, T.-H. Arima, T.
Saerbeck, T. Hanashima, A. Sitnikova, D. Kirilenko,
N. Yakovlev and N. Sokolov, Sci. Rep. 8, 8741 (2018).
[3] Y. Sakaguchi, T. Hanashima, H. Aoki, H. Asaoka, A.
Simon and M. Mitkova, Phys. Status Solidi A 215,
1800049 (2018).
[4] K. Sakurai, M. Mizusawa, J. Jiang and T. Ito, Physica

B: Condensed Matter 551, 426–430 (2018).
[5] R. Maruyama, D. Yamazaki, K. Akutsu, T. Hanashima,
N. Miyata, H. Aoki, M. Takeda and K. Soyama, Nuclear
Inst. Meth. Phys. Res., A888, 70–78 (2018).
[6] S. O.-Kawamura, T. Hattori, S. Harjo, K. Ikeda,
N. Miyata, T. Miyazaki, H. Aoki, M. Watanabe, Y.
Sakaguchi and T. Oku, Neutron News 30, 11–13(2019).
[7] T. Miyazaki, N. Miyata, M. Asada, Y. Tsumura, N. Torikai,
H. Aoki, K. Yamamoto, T. Kanaya, D. Kawaguchi and
K. Tanaka, Langmuir 35, 11099–11107 (2019).

N. Miyata1, H. Aoki2,3, K. Soyama4, D. Yamazaki2,5, K. Akutsu1, T. Hanashima1, and S. Kasai1
Neutron Science and Technology Center, CROSS; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center; 3Instituteof Materials Structure Science, KEK; 4Materials and Life Science Division, J-PARC Center; 5Neutron Instrumentation Section, Materials andLife Science Division, J-PARC Center

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Status of SENJU 2018
1. Introduction
SENJU is a TOF single-crystal neutron diffractometer designed for precise crystal and magnetic structure
analyses under multiple extreme environments, suchas low-temperature, high-pressure and high-magnetic
field, as well as for taking diffraction intensities of small
single crystals with a volume of less than 1.0 mm3 down
to 0.1 mm3 [1]. Ever since SENJU was launched in 2012,
continuous commissioning and upgrading operations
have been carried out.
In 2018, we installed a new vacuum sample chamber for the future’s installation of additional detectors,
and successfully established the fine-calibration method of the detector position. In addition, we also reporton the purposes for which the instrument beam-time
for SENJU was used.
2. Installation of a new vacuum sample chamber
The detector arrangement of SENJU is almost cylindrical, 36 detectors are arranged cylindrically aroundthe sample position and only one detector is positioned
at the bottom of the sample position. Consequently, theobliquely downward direction of the sample position is
not covered by the detector and the reciprocal spacearound the azimuth region of the f-axis was not measured without pulling out the goniometer and changing
the sample orientation. To solve this problem, we havea plan to add detectors. As the first step of this plan,
we manufactured and installed a new vacuum sample

Figure 1. Schematic view of the new vacuum sample chamber and the detector arrangement. Blue boxes in
the figure show the present detector arrangement
and red boxes show the new detectors that will be
installed in near future.

102

chamber. The new chamber has a dome-shaped basement made from aluminum. The thickness of the domeis 5 mm. The additional detectors will be set up in near
future, as shown in Fig. 1.
3. Fine calibration of the detector position
For single-crystal diffractometers, the ability to accurately determine the lattice constants of materials
is one of the most important requirements, since thechanges of lattice parameters are often indicative ofphase transitions and bond lengths, which are directory
related to the lattice parameters, determines the chemical properties. The accuracy of the lattice parameterslargely depends on the accuracy of the instrumental
parameters that define the positions of each detector
with respect to the sample position and the incident
beam. Therefore, the determination of the instrumental
parameters, in other words “calibration”, is very essential
for the operation of instruments. Nevertheless, there isno established way to determine the instrumental parameters, and thus we developed a systematic procedure for calibration of SENJU.
There are 37 2D-detectors installed on SENJU. One
module is composed of vertically aligned 3 detectors(top, middle and bottom), and 12 modules are cylindrically placed around the sample position (the restof one detector is located underneath the sample position). 7 parameters for each detector describing thegeometrical location of the detector and the distance
between the target and the sample position (L1) haveto be determined (260 parameters in total). The calibration procedure was divided into two parts: the part todetermine the parameters for the middle detectors andthe part for the rest of detectors in order to avoid biases
as much as possible. In the procedure, a single crystal of
C12A7 (Maynite: 12CaO•7Al2O3) was used as a standard
sample. The structure of this material is cubic, and thelattice constant was precisely measured by X-ray in advance (a  12.0018 Å).
The sample was mounted on a one axis (omega)goniometer in a way that c-axis is aligned with the rotation axis (vertical axis). Under these conditions, numberof Bragg reflections of (h k 0) can be measured on the
middle detectors. By rotating the sample in small-angle
steps such as 0.5°, the same Bragg reflections can bemeasured on the same detectors number of times anda series of Bragg reflections forming a line can be obtained. In addition, another series of Bragg reflections

MLF Annual Report 2018(h k 0) can be measured by doing the same measurements after rotating the sample by 180°. Here, two linesof Bragg reflections have been recorded on the middle detectors, as shown in Fig. 2, as well as many other
Bragg reflections on other detectors.
As the first part of the calibration, the distance between the sample and the detectors and the positionof the equator on the detectors are calculated from theintervals of the Bragg reflections in the series and thegap between the two lines, respectively. Provided theseparameters and the lattice parameters are fixed, the rest60

y (pixel)

50
40
30
20
10

10

20

30

x (pixel)

40

50

60

Figure 2. A typical example of a series of Bragg reflections
measured during the calibration measurement byrotating the sample in small-angle steps.

Neutron Scienceof parameters of the middle detectors and the orientation of the sample are determined based on the leastsquare method. By this process, all the parameters ofthe middle detectors and the orientation of the sample,
that is the UB-matrix, are determined.
As the second part of the calibration, the parameters of the rest of the detectors are refined based on
the least-square method to best match the positions of
the observed Bragg reflections and the predicted positions based on the UB-matrix. The flight path (L1) is also
refined simultaneously in this process.
All the processes mentioned above are integrated
into one program, thus once the necessary measurements are conducted, the calibration will be done justby inputting the data into the program. One thing to be
noted is that some parameters are not sensitive enoughto be precisely determined with this process, thus further improvement is required.
4. Use of the instrument beam-time
In 2018, the instrument beam-time was used mainly for measurements of standard samples, a vanadiumnickel alloy for calibration of the detector efficiency. In
addition, we used the instrument beam-time to compensate beam-time of some general-use proposals lost
due to usage problems of sample environment devices.
Reference[1] T. Ohhara et al., J. Appl. Cryst., 49 120 (2016).

T. Ohhara1, R. Kiyanagi1, A. Nakao2, K. Munakata2, Y. Ishikawa2, K. Moriyama2, I. Tamura1, and K. Kaneko1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science and Technology Center, CROSS

1

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TAKUMI and the Engineering Sciences
1. Introduction
TAKUMI is a neutron diffractometer dedicated forresearch in engineering materials sciences, which was
installed at beamline 19 in the MLF of J-PARC. Carefulanalysis of the Bragg peaks in a neutron diffraction pattern can reveal important structural details of a sample
material, such as internal stresses, phase conditions,dislocations, texture, etc. Experiments in TAKUMI varyfrom internal strain mapping in engineering components, microstructural evolutions during deformationsof structural or functional materials at various temperatures, microstructural evolutions during manufacturing(thermo-mechanical) processes, to texture analyses ofengineering materials.
TAKUMI has entered its 10th year since the startof commissioning. Many fruitful results using various
materials from different engineering fields have beenobtained through users experiments, internal project
researches and instrumentation activities. Various sample environmental devices have been also developed
independently by the TAKUMI team or together withusers to realize numerous types of materials engineering experiments using neutron diffraction ex situ or insitu. They include several loading machines for highand low temperatures, as well as for room temperature,
furnaces, a cryostat, a simulator for thermo-mechanicalprocess (thermec-mastor), a cradle, radial collimators,
and so on. Different kinds of data analyses have been
also established to obtain the above structural detailsof the sample materials.
2. Statistics of experiments and sciences
In FY2018, thanks to users and collaborators, wewere able to conduct various experiments, and several
excellent refereed papers have been published. The
experimental type statistics done during FY2018 areshown in Fig. 1. The experiments cover ex situ measurements, including strain mappings and diffraction measurements of samples with histories of deformations
and/or heat treatments, and in situ measurements including loading experiments at temperatures covering
1273 K to 10 K, measurements during applications of acyclic electric field, and so on.
Many excellent papers have been published in
FY2018, and the highlighted ones are as follows:a. “Deformation behavior of as-cast and as-extruded
Mg97Zn1Y2 alloys during compression, as tracked byin situ neutron diffraction”, by Wu Gong et al. [1]. The
104

Figure 1. The experimental type statistics done during
FY2018 in TAKUMI.

yield strength of Mg97Zn1Y2 alloy, containing a long
period stacking ordered (LPSO) phase and an α-Mgphase, was found to be substantially enhanced by
hot extrusion. The quantitative evaluation of phasestress partition confirmed that the LPSO phase wassignificantly enhanced by hot extrusion and kinkdeformation of the LPSO phase plays an importantrole in preserving ductility.
b. “In situ Neutron Diffraction Study on Ferrite andPearlite Transformations for a 1.5 Mn-1.5 Si-0.2 C
Steel”, by Yo Tomota et al. [2]. In situ neutron diffraction enables us to investigate the changes inlattice constants of ferrite and austenite, which areaffected not only by thermal contraction but also
by transformation strains, thermal misfit strains,and carbon enrichment in austenite. Pearlite
transformation started after carbon enrichment inaustenite reached approximately 0.7mass% andcontributed to the broadening of the diffraction
line.
c. “Deformation of CoCrFeNi high entropy alloy atlarge strain”, by Bing Wang et al. [3]. A three-stage
deformation behavior was fully captured by latticestrain and texture evolution. In spite of the chemical complexity, the deformation in CoCrFeNi is
dominated by dislocation activities. Analysis of diffraction and microscopy data shows that the deformation progresses from dislocation slip to severe
entanglement, where a sharp increase in dislocation density is observed.

MLF Annual Report 2018

d. “Stroboscopic time-of-flight neutron diffraction
during cyclic testing using the event data recording system at J-PARC”, by Takuro Kawasaki et al. [4].
A time-resolved time-of-flight neutron diffraction
technique to characterize the structural propertiesof materials during cyclic tests has been developed
for the neutron diffractometers at J-PARC. Using
this technique, diffracted neutrons and the applied
cyclic conditions are recorded as event data together with time information. The developed techniqueenabled the collection and processing of diffraction
data for all levels of the applied electric field, as opposed to only the highest and lowest levels.
e. “High stereographic resolution texture and residual stress evaluation using time-of-flight neutron
diffraction”, by Pingguang Xu et al. [5]. Pole figure
evaluation of a limestone standard sample with awell-known texture suggested that the precisionobtained for texture measurement is comparable
to that of the established neutron beamlines utilized for texture measurement, such as the HIPPO
diffractometer at the Los Alamos Neutron Science
Center (New Mexico, USA) and the D20 angledispersive neutron diffractometer at the Institut
Laue–Langevin (Grenoble, France). A high-strength
martensite–austenite multilayered steel was employed for further verification of the reliability ofsimultaneous Rietveld analysis of multiphase textures and macro stress tensors.
3. New sample environmental devices
To understand the mechanism of grain refinementof metallic materials by thermo-mechanical process, ourcollaborators from Kyoto University developed a compressive loading device equipped with an induction
heating system, called the thermec-mastor, enablingheating and cooling with fast rates (30 K/s), as well as afast deformation rate (100 mm/s) [6]. The loading axis of
the thermec-mastor can be, however, aligned vertically,measuring only the scattering vectors parallel to the radial direction of specimen. On the other hand, changes
in the lattice parameters in the loading direction of thespecimen are crucial to explore the internal stresses, aswell as atomic partitioning during thermo-mechanical

Neutron Science

processes. To answer these demands, we developed
a new sample environmental device for horizontal
loading equipped with an induction heating system.
The sample area of the new sample environmental
device is shown in Fig. 2. The new device is still undercommissioning.

Figure 2. The sample area of a new sample environmental
device for horizontal loading equipped with an induction heating system.

4. Future plans
We have developed and/or established many sample environmental devices as well as measurement and/or analyses methods. In the future, we will focus mainly
on conducting engineering research together with ourcollaborators and users. In the same time, we will also
continue to upgrade TAKUMI, which will include introducing new devices and further method development,
taking into account the trends in engineering research.
References[1] W. Gong et al., International Journal of Plasticity
111, 288–306 (2018).
[2] Y. Tomota, et al., ISIJ International 58, 2125–213(2018).
[3] B. Wang et al., Scripta Materialia 155, 54–57 (2018).
[4] T. Kawasaki et al., Journal of Applied Crystallography51, 630–634 (2018).
[5] P.G. Xu et al., Journal of Applied Crystallography 51,
746–760 (2018).
[6] A. Shibata et al., Scripta Materialia 165, 44–49(2018).

S. Harjo1, T. Kawasaki1, and K. Aizawa2
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Technology Development 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, local government of Japan’s 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 that could be used by materials engineers andscientists in their materials development work, including chemical analytical instruments.
The applications of neutron diffraction in materials science are designed (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 andimprovements of functions, especially for practical materials. A diffractometer with super high resolution is
not required to achieve those goals. The match of features like intermediate resolution around d/d  0.15%,
high intensity and wide d coverage is more important.
This diffractometer is designed to look at a decoupled-poisoned liquid hydrogen moderator (36 mm, offcentered) (BL20), and it has an incident flight path (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 are listed in Table 1.
There are four detector banks, including a low-angle

Figure 1. IBARAKI Materials Design Diffractometer, iMATERIA
without detector for each bank and instrument
shielding. The high-resolution bank, special environment bank (90°-bank), and low-angle bank, canbe seen from right to left. The small-angle detectorbank, which is not shown in the picture, is situatedin the low-angle vacuum chamber (left-hand sideof the picture).

106

Table 1. Instrumental parameters of iMATERIA. L2 is the scattered flight path. The d-range (q-range) for eachbank is the maximum value for the 2-measurement
mode.

L1
26.5 mGuide length
Position of Disk choppers

HighResolution
Bank
SpecialEnvironment
Bank
LowAngle
Bank
SmallAngle
Bank

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

Total 14 m (3section)
7.5 m (double)
11.25 m (single)
18.75 m (single)
150°  2θ  175
2.0 – 2.3 m
0.09  d (Å)  5.0°
80°  2θ  100°
1.5 m
0.127  d (Å)  7.2
10°  2θ  40°
1.2 – 4.5 m
0.37  d (Å)  58
0.7°  2θ  5°
4.5 m
0.007  q (Å1)  0.6

and small-angle scattering detector bank. The angularcoverage of each detector bank is also shown in Table 1.
The rotation speeds for the disk-choppers are the same,with a pulse repetition rate of 25 Hz for most applications (SF mode). In this case, the diffractometer covers
0.18 d (Å) 2.5 with d/d  0.16% and covers 2.5 d (Å)
800 at three detector banks of 90°, low-angle andsmall-angle with gradually changing resolution. Whenthe speed of the wavelength selection disk-choppers
is reduced to 12.5 Hz (DF mode), we can access a wider
d-range, 0.18 d (Å) 5 with d/d  0.16%, and 5 d (Å)
800 with gradually changing resolution and doubled
measurement time compared to the SF mode.
2. Current status
All four banks, high-resolution bank (BS bank),
special environment bank (90° bank), low-angle bankand small-angle bank, are operational. It takes about 5
minutes (in DF mode) to obtain a ‘Rietveld-quality’ datain the high-resolution bank at 500-kW beam power for
about 1 g of standard oxide samples.
Figure 2 shows a typical Rietveld refinement pattern for a LiCoO2 sample, cathode material for lithium
ion batteries (LIB), at the high-resolution (BS) bankby the multi-bank analysis function of Z-Rietveld [2].
It takes 20 min in DF mode to collect the available

MLF Annual Report 2018

Figure 2. Rietveld refinement pattern for LiCoO2 at the highresolution bank of iMATERIA.

Rietveld data, due to the high neutron absorption crosssection for natural Li (sNat 70 barn).
3. Sample Environments
The automatic sample changer is the most important sample environment for high-throughput experiments. Our automatic sample changer [3] consists of asample storage, elevating system of two lines, two setsof pre-vacuum chambers and a sample sorting system.

Neutron Science

We can handle more than 600 samples continuously atroom temperature without breaking the vacuum of thesample chamber.
The V-furnace (900°C), the gas-flow furnace(1000°C), the cryo-furnace (4K) and the 1K cryo are
ready for experiments. The in-operando experiment
system for LIB with a sample changer is available in cylindrical and coin types of batteries.
The rapid heating/quenching furnace with an automatic sample changer (RT – 1273 K with heating speed
10 K/s and cooling speed >20 K/s) and the universal deformation testing machine (max loading 50kN with RT– 1273 K) are available for texture measurement.
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. Hoshikawa, T. Matsukawa, and Y. Onuki
Frontier Research Center for Applied Nuclear Sciences, Ibaraki University

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Online Analysis System for NOVA
1. Introduction
The High-intensity neutron total diffractometer(NOVA) is able to measure the static structure factor S(Q)with high precision in a very short time. The pair-distribution function G(r) derived from the Fourier transformof the S(Q), is used for the structure analysis of disordered materials, such as liquid, glass, amorphous and soon. The expected neutron intensity at NOVA is approximately 0.34  108 neutrons/s·cm2 · MW [1], and as common use, the neutron intensity is the most intense at
MLF. NOVA is a wide-Q range machine to measure disordered material structures and is also a high-intensity
powder diffractometer to measure crystalline material
structures (Q/Q0.35%). To figure out the experimental status at NOVA, an online monitor is a very usefultool. We developed a new online monitor modified
with the current data acquisition (DAQ) system. In thisreport, we will describe the new tool.
2. DAQ-Middleware
DAQ-Middleware (DAQ-MW) [2] is a framework torealize the DAQ system in a network distributed environment easily and is standard DAQ software at MLF. DAQMW is able to integrate some DAQ machines in a network
distributed environment. DAQ-MW is based on Robot
Technology (RT) Middleware [3]. Users can customize
the system configuration according to their requirements. The typical system configuration for DAQ-MW
is shown in Fig. 1. DAQ-MW consists of a management
part, including Daq Operator, and a function part, which
includes a Gatherer component, Dispatcher component,

Logger component and Monitor component. The functions of each component are shown in Table 1. Eachcomponent is designed as a state machine, and definedsystem control actions depending on the statements(‘Load’, ‘Configure’, ‘Running’, ‘Pause’). The transition between the statements is carried out by control commands such as ‘Configure’, ‘Unconfigure’, ‘Begin’, ‘End’,‘Pause’ and ‘Resume’. DAQ components are connectedwith its input and output ports, for instance, the simplest DAQ system, which is constructed from Gatherer
and Logger components, is can be created. The datatransportation between the DAQ components is supported by Common Object Request Broker Architecture(CORBA) [4]. Since CORBA has a common interface definition language, it makes possible the data transportation
between different computer languages and different
operating systems. In general, since CORBA’s processing overhead is bigger , the data transportation is lesseffective than that of Transmission Control Protocol andInternet Protocol (TCP/IP). By increasing the data size at
one time, the performance will become closer to that of
TCP/IP. DAQ-MW has two types of the parameter-set algorithm, and some parameters are written in parameter

Table 1. The functions of each component.

Gatherer

Connecting with read-out modules

Dispatcher

Splitting data flow

LoggerData logging on the storage

MonitorOnline data processing

Figure 1. The typical system configuration for DAQ-MW.

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files as Extensible Markup Language (XML) or JavaScript
Object Notation (JSON). Those parameter-set algorithms
are distinguished by the frequency of use. The system
configuration will be set at one time when the DAQ machine restarts. On the other hand, the equipment andanalysis parameters will be set after every ‘Configure’
statement. Since DAQ-MW has a Graphical User Interface(GUI) control panel, which runs on a web browser, we
can control DAQ-MW via the network.
3. Improvement of DAQ-MW
Though DAQ-MW has been stably working at NOVA
for several years, there are still some weak points in the
online data processing. Since DAQ-MW is a tightly coupled system connected with some DAQ components, it
is good at treating some regular tasks and not suitableto deal with an irregular task, such as a histogram drawing which is increasing CPU load gradually. Therefore,
once Monitor component takes a long time to draw ahistogram, the DAQ system will be down because ofblock data flow. Thus far, the measurement data has
been usually decimated to keep the stability of the DAQ
system during the online data processing. In order tomonitor the experimental status within a short time,
online data processing for all data (Live Data Reduction:
LDR) is required. In the other large facility such as SNS
and ESS, the development of LDR has already started.
Therefore, we also started to develop a loosely coupledsystem to overcome our weak points. For our purpose,
we applied redis [5] which can create Key-Value Store(KVS). Since KVS has a simple data structure of ‘Key’ andNeutron Science‘Value’, it’s useful to construct a database, which meetsthe requirement for handling a huge amount of data. A
redis server works fast on computer memory. The datatypes such as a string type, a list type and so on, are used
as a data type of ‘Value’. And redis supports several computer program languages, such as C/C, Python, Ruby
and so on. Since redis is an open source program, theinstallation cost will be minimal. A redis server is used
not only as a simple queue server (queue model), butalso as a broker for publish-subscribe model. The typical usage of a redis server is shown in Fig. 2. The queue
model is corresponding to one-to-one connection system, and some data setting into a redis server are kept
until picking up. The stored data size is limited by theamount of computer memory. On the other hand, thepublish-subscribe model is corresponding to an N-to-N
connection system, if no subscribers are registered,
the published data will be erased. As shown in Table 2,since the publish-subscribe model is also a spatially,
temporally and synchronously separated system, thosecharacteristics play an important role in improving theonline data processing capability.
The new system configuration for DAQ-MW isshown in Fig. 3. Two new DAQ components, Publisher
and DaqInfoPublisher, which use redis publish-subscribe model, have replaced the old Monitor component. The Publisher component publishes measurement
data from the readout modules to a redis server. The
DaqInfoPublisher component publishes the DAQ status, such as ‘Begin’, ‘End’ and so on to a redis server. A
redis server, which is regarded as a large scale and fast

Table 2. The characteristics of redis publish-subscribe model.

Spatially

A publisher and a subscriber can be located anywhere in the network.

Temporally

Anytime, a publisher is able to publish, and a subscriber is able to subscribe.

Synchronously

A publisher and a subscriber can register and leave.

Figure 2. The typical usage of a redis server: (left) queue model, (right) publish-subscribe model.

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MLF Annual Report 2018

Figure 3. The new system configuration for DAQ-MW.

data buffer, plays an important role to separate clearly
LDR from the DAQ system. A subscriber program subscribes some information, such as measurement data
and the DAQ status, from a redis server. And a subscriber, which is the core program of LDR, is able to operatea higher CPU load task without blocking the DAQ system. Since a subscriber program obtains the DAQ statusfrom a redis server, the DAQ system and a subscriber
program works synchronously. The simple online monitor is created by JSROOT [6]. The time-of-flight distributions, the beam profile, the trend graphs and so on aredisplayed in the simple online monitor. Users can accessthe simple online monitor via network, and then obtain
images of some histograms, change display conditions,and read statistic information.

Acknowledgement
This work was performed under the S1-type program (2014S06) approved by the Neutron Scattering
Program Advisory Committee of IMSS, KEK.
References[1] H. Ohshita, et al., JPS Conf. Proc. 8 (2015) 036019.
[2] K. Nakayoshi, et al., Nucl. Instr. and Meth. A 623(2010) 537.
[3] Object Management Group, Specification of
Robotic Technology Component (RTC), Version 1.0,
http://www.omg.org/spec/RTC/1.0/.
[4] web page of CORBA, http://www.corba.org.
[5] web page of redis, http://redis.io.
[6] web page of JSROOT, https://root.cern.ch/js.

H. Ohshita1,2, K. Ikeda1,2,3, T. Honda1,2,3, T. Otomo1,2,3,4, Y. Yasu1, T. Seya1,2, N. Kaneko1,2, K. Suzuya2, S. Sashida3, and M. Tsunoda4
Institute of Materials Structure Science, KEK; 2Neutron Science Section, Materials and Life Science Division, J-PARC Center; 3SOKENDAI;
4Graduate School of Science and Engineering, Ibaraki University

1

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Neutron Science

Status of the Energy-Resolved Neutron Imaging System
RADEN
1. Introduction
The energy-resolved neutron imaging system“RADEN”, installed at beamline BL22 in the Materials
and Life Science Experimental Facility (MLF) of J-PARC,
is a dedicated instrument for conducting wavelength/
energy-dependent neutron imaging experiments withfull utilization of the short-pulsed neutron’s nature,such as broad available neutron energy range and narrow pulse shape [1]. RADEN has the capabilities to conduct the energy-resolved neutron imaging techniques,
such as Bragg-edge, neutron resonance absorption,and polarized pulsed neutron imaging. In addition, thewavelength dependence analysis has been combinedwith the neutron phase imaging based on a Talbot-Lau
interferometer by using pulsed neutrons [2]. In this report, we will cover the current status of RADEN’s activities, including technical developments and application
studies.
2. User programs
RADEN is accepting about 30 user programs every
year, and more than half of them are using the energyresolved neutron imaging technique. Especially thestrain distribution measurement in metallic alloy samples made by the additive manufacturing technique is
one of the increasing application studies of Bragg edge
imaging. In addition, intensive developments in combining computed tomography and energy-resolved
imaging have been carried out. Also, visualization of
three-dimensional strain distribution in a deformed steel
sample [3, 4] and magnetic field strength and direction

generated in a small solenoid coil [5, 6] have been done.
Another application that attracts attention is in-situ observation of the crystal growth process. Owing to thehigh penetration power of neutrons, it is possible toobserve the solid/liquid interface directly through thefurnace and to control the interface shape precisely during the observation, which is important in producing ahigh-quality crystal without defects or composition inhomogeneity [7]. Moreover, the neutron resonance absorption technique helps to quantitatively visualize the
distribution of dopant element during the growth. This
study is expected to accelerate the decisions necessary
to make during the crystal growth process.
On the other hand, the demand for neutron imaging of objects, including large neutron absorption elements like Boron, has been increasing recently. Because
RADEN can provide enough neutron intensity with energy larger than 1 eV, it is possible to obtain good transmission for such an object. To fulfil those requests, we
conducted epi-thermal neutron imaging with parking
the T0 chopper open and inserting Cd filter in the beam
path to eliminate thermal and cold neutrons.
3. Development and improvement of the neutron
imaging technique
High-spatial resolution imaging experiments havebeen demonstrated by means of the center-of-gravity
technique using an MCP detector [8]. With this highspatial imaging mode, 16 m spatial resolution could beobtained, which was 4 times smaller than the pixel sizeof MCP detector of 55 m (Fig. 1). The same techniqueFigure 1. Results of the high-resolution imaging experiment. Photograph of the MCP detector and the test target(left), obtained image with coarse collimation (L/D=298) (center), and image with fine collimation (L/D=667)(right). It is possible to recognize the space smaller than 20 μm with a fine collimation condition.

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Figure 2. An illustration of polarized neutron phase imaging setup.

Figure 3. Results of the polarized phase imaging experiment. A photograph and a schematic illustration of samples (A), (B).
Obtained differential phase image using polarized neutrons with positive spin polarity (C) and with negative spinpolarity (D).

is going to be adapted to the normal neutron radiography using a CMOS camera. Next, the excessive time
for a CT measurement has been improved drastically by
a new dedicated measurement system composed of apulse counter and a rotation stage controller. With thissystem, the required communication time between thecontrol software and devices has been reduced to a few
seconds. As a result, a typical CT measurement finishes
in several hours.
Finally, the Talbot-Lau interferometer for thepulsed neutron phase imaging has been developed
at RADEN [2]. Because a phase shift of a neutron wave
depends on the neutron wavelength, the use of wavelength dependence analysis is beneficial to its accurate
and precise evaluation. Moreover, the neutron phaseimaging is sensitive to a magnetic field, since the phaseshift occurs by optical potentials produced by nuclei
and magnetic fields. Hence, we tried to use polarizedneurons to detect magnetic information. Because thesign of the magnetic potential depends on the neutron
polarity, unlike the nuclear potential, differential phase
images obtained with flipping the spin polarity of a polarized neutron and subtracting each other enables us
to extract the magnetic contribution. An illustration of112

the polarized neutron phase imaging set up is shownin Fig. 2. With this apparatus, we obtained successfully
different contrast images by changing the neutron spinpolarity for magnetic samples (Fig. 3).
4. Summary and future plans
Now, RADEN is under user operation and the application fields spread widely in both scientific and industrial disciplines. Especially the number of proposals
about in-situ or in-operando observation experiments
are increasing. Owing to the continuous improvement
work, the basic imaging techniques become more sophisticated with every passing year. Also, we are developing new imaging techniques utilizing wavelength/
energy dependence. In the near future, the energyresolved neutron tomography is expected to become
a general technique at RADEN, which visualizes thethree-dimensional distribution of strain, magnetic field,
elemental composition, and temperature.
Acknowledgements
This work was partially supported by the JST ERATO
Momose Quantum Beam Phase Imaging Project.

MLF Annual Report 2018

References[1] T. Shinohara et al., J. Phys: Conf. Series 746 012007(2016).
[2] Y. Seki et al., Europhys. Lett. 123, 12002 (2018).
[3] J. N. Hendriks et al., Phys. Rev. Materials 1 053802(2017).
[4] A.W.T. Gregg et al., Phys. Rev. Applied 10 064034

Neutron Science(2018).
[5] M. Sales et al., Scientific Reports 8 2214 (2018).
[6] M. Sales et al., J. Phys. D: Appl. Phys. 52 205001(2019).
[7] A. S. Tremsin et al., Crystal Growth & Design 17 6372
(2017).
[8] A. S. Tremsin et al., Nucl. Instr. Meth. A 787 20 (2015).

T. Shinohara1, T. Kai1, K. Oikawa1, M. Segawa1, T. Nakatani2, K. Hiroi1, Y. Su2, H. Hayashida3, J. D. Parker3, Y. Matsumoto3, Y. Seki1,
and Y. Kiyanagi4
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Technology Development Section, Materials and Life Science
Division, J-PARC Center; 3Neutron Science and Technology Center, CROSS; 4Graduate School of Engineering, Nagoya University

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MLF Annual Report 2018

On-Beam Commissioning on POLANO
1. Introduction
One of the remaining challenges in the pulsed neutron technique is the realization of polarization analysis,
particularly with inelastic scattering. It is a promisingtechnique that can be used for the recent research in
the field of material science with entangled degrees
of freedom. In order to accomplish advanced neutron
experiments using intense pulsed neutrons at theMaterials and Life Science Experimental Facility (MLF),
J-PARC, POLANO has been dedicated for use as a polarization beam line. POLANO is a chopper type spectrometer with polarization analysis capability and is
now under construction at the MLF [1–5]. The design
and manufacture of the main components were completed by 2016. In 2016, the radiological assessment for
acceptance of neutron beam was successfully conducted. Consequently, POLANO was approved as a proper
neutron beam line and the on-beam commissioning
process for future scientific program use has alreadystarted.
Our primary motive for designing POLANO is toachieve higher-energy polarization analysis of inelastic scattering beyond a reactor-based neutron source.
A wide momentum and energy region are necessary toprovide the research opportunities in the field of multiple degrees of freedom. Our final objective is to obtainup to 100 meV of the transfer energy and around 10 Å1
in momentum space.
2. Spectrometer design
POLANO is located at BL23 in MLF, viewing the hydrogen decoupled moderator. The geometrical parameters of the spectrometer are as follows: distance frommoderator to sample L1, distance from sample to detector L2, and distance from Fermi chopper to sample
L3 are 17.5 m, 2.0 m, and 1.85 m, respectively. In orderto gain more space after the Fermi chopper, a long L3 isused, without losing much resolution. An energy resolution of E / Ei  3 to 5% and momentum resolution ofQ / ki  1 to 2% were achieved. These values are sufficient for observing most of the magnetic excitationsin the so-called strongly correlated electron systems,
where the magnetic excitations are scaled by exchangeor super exchange coupling constant J  100 meV. A
resolution of a few meV could be enough to see the detailed structures even at higher incident energy. Also, inorder to observe the incommensurate structure in cuprate high-Tc superconductors, the incommensurability
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is in the range of a tenth in reciprocal lattice unit, whichcorresponds to the order of 0.1 to 0.2 Å1. The incommensurate structure can be observed separately with
our resolution.
After passing the moderator, the neutrons aretransported by supermirror guide tubes with m  4,
optimized for around 110 meV neutron intensity with a
McStas simulation [6, 7]. An elliptical guide, which is optimized section wise (section length  50 cm) can yielda neutron flux of 3.9  105 [n/sec/meV/cm2/MW], whichis almost comparable with a coupled moderator beamline at E  100 meV.
A SEOP 3He filter cell will be placed at L  16.435 m
from the moderator. The 3He filter has a beam width of
8 cm at the bottom, and 4 cm at the half height. In theearly stages, 3He cells with a diameter of 5 cm will be
used, because the 3He polarizing technique has alreadybeen established for 5 cm cells [8].
3. On-beam Commissioning
In 2018, we started on-beam commissioning on
POLANO in order to evaluate all the devices and instruments and ensure that they operate properly. Figure 1
depicts the neutron beam cross section at POLANO
sample position both simulation (left) and measurement (right). In the left upper panel different valuesof neutron energy from 5 to 200 meV were taken into
account for the simulation. The lower panel depicts

Figure 1. (left) Simulated beam cross section at sample position. (right) Measured neutron intensity by imaging
plate.

MLF Annual Report 2018

one-dimensional integrated intensity along horizontal
position. Comparison of the simulation and measurement data shows that the 1D peak profiles are very similar to each other. The peak width of the measured 1D
peaks on both horizontal and vertical can be well reproduced by the simulation. Transportation designing with
4 Qc supermirror guide tube is, thus, successfully tested
by using neutron beam. The transported neutron intensity (absolute flux) is measured in two different ways:
by using gold foil, and also using 3He detectors. The
corrected values of these two absolute fluxes are evaluated 1.58  108 and 3.3  108 [n/cm2/s/MW] for gold-foiland 3He detectors, respectively. The neutron energy dependence of the measured flux is in good agreementwith that calculated by McStas Monte Carlo simulation.
Thus, the neutron transportation ability on POLANO
is assessed by on-beam test as we expected on guidetube designing.
Figure 2 shows the neutron scattering data measured on a real material CsVCl3, which is known as a onedimensional (1D) quantum spin magnet. CsVCl3 has S
 3/2 spins arranged antiferromagnetically along c-direction. Those spins are 3D ordered at low temperature
TN  13.3 K [9,10]. In order to see the dynamics of the
1D spin chains, the inelastic spectrum at T  20 K was

Figure 2. The first inelastic signals by the POLANO spectrometer.

Neutron Sciencemeasured with “unpolarized” neutrons. In addition to
the phononic excitation lying at lower energy, a clearlyobserved palm tree structure originated from magnetic
1D chains at Q1D  1.0 and 3.0, which corresponded to
the 1D magnetic first and second Brillouin zone center.
4. Future plans
We have to seriously consider unexpected contaminations (background) when analyzing the data. We
plan to install a direct beam catcher, and collimators to
reduce that accidental scattering. Polarization analysis
is of course the main purpose of this instrument. We arecontinuing our efforts to make possible the polarization experiments in the near future. R&D of the crucial
devices as SEOP polarizer and magnetic guide fieldsystem are now in the final stage of installation at thebeam line [11].
References[1] T. Yokoo, et. al., J. Phys. Soc. Jpn. 82 (2013) SA035.
[2] K. Ohoyama, et. al., J. Phys. Soc. Jpn. 82 (2013)
SA036.
[3] T. Yokoo, et. al., Journal of Physics Conf. Series 502(2014) 012046.
[4] T. Yokoo, et. al., EPJ Web of Conferences 83 (2015)
03018.
[5] T. Yokoo, et. al., AIP conference proceedings 1969(2018) 050001.
[6] K. Lefmann and K. Nielsen Neutron News 10/3
(1999) 20.
[7] P. Willendrup, E. Farhi, K. Lefmann, Physica B 350(2004) 735.
[8] T. Ino, et. al., ibid.
[9] H. Kadowaki, et. al., J. Phys. Soc. Jpn. 52 (1983)
1799.
[10] S. Itoh, et. al., Phys. Rev. Lett. 74 (1995) 2375.
[11] N. Kaneko, et. al., ibid.

T. Yokoo1,2, N. Kaneko1,2, Y. Ikeda3, S. Itoh1,2, M. Fujita3, M. Ohkawara3, T. Ino1,2, and K. Hayashi1
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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MLF Annual Report 2018

3

He Neutron Spin Filter Cells

1. Introduction
A polarized 3He neutron spin filter (NSF) is a key
component in POLANO [1]. An in-situ polarized 3He
NSF functions as the incident neutron beam polarizer,
where 3He gas is continuously spin-polarized on the
instrument by spin-exchange optical pumping (SEOP)
to obtain steady neutron beam polarization. Anotherpolarized 3He gas will be employed for the spin-analysis of the scattered neutrons on the next stages of the
POLANO project. To achieve the best quality of neutron
polarization or neutron spin-analyzing power, the highest 3He polarization as well as a very long spin relaxation
time of polarized 3He gas is of great importance. One of
the crucial techniques in 3He gas polarization by SEOP
is manufacturing of high quality 3He gas container cells.
In SEOP, alkali metal atoms are polarized by opticalpumping, and the angular momentum of polarized alkali
atoms is transferred to 3He nuclei by hyperfine interaction [2]. The alkali metals are confined in a container cellwith 3He gas, and the cell is heated to 200–250°C to maintain appropriate alkali number density. Listed below aresome of the essential requirements for such SEOP cells:(1) Transparent to the optical pumping light.
(2) Transparent to neutrons.
(3) No helium leakage.
(4) No magnetic impurities.
(5) Alkaline resistant in high temperatures.
(6) Tolerate high pressure.
Aluminosilicate glass containing no boron can be
the only candidate material for SEOP cells today. Single
crystals [3] or transparent ceramics can be an alternative choice, but cells made of these materials can hardly
satisfy all the requirements.
2. Fabrication of GE180 cells
We use a type of aluminosilicate glass named
GE180 to fabricate SEOP cells. This aluminosilicate glass
fulfills all the above requirements, and almost all the
SEOP cells used today all over the world are made ofthis material. Spin-relaxation times of polarized 3He gas
in GE180 cells can occasionally approach the theoreticallimit; 3He polarizations of more than 80% are regularly
achieved. The only drawback of using GE180 is glassblowing, which is very difficult to work with. Comparedto Pyrex, commonly used glass in scientific researches,
the softening temperature of GE180 is higher, and theworking temperature range, where the glass keeps appropriate viscosity for glassblowing, is narrower.
116

We have been making SEOP cells using GE180 in acollaboration between J-PARC and Tohoku University.
Shown in Fig. 1 is one of our SEOP cells, glassblowing by
Mr. Tomomi Kudo of Tohoku University (Fig. 2) and 3He
gas filling at KEK. The cell contains 3He gas of 3.4 atm topolarize 100 meV neutrons. The glass cell was designed
using the finite element method so as to withstand aninternal gas pressure of 6 atm, which is expected during the optical pumping at 250°C.
A blown GE180 cell is attached to the string partmade of Pyrex that is to be connected to a high vacuum
system for the gas filling (Fig. 3). GE180 and Pyrex tubes
are connected together using glasses that have thermal expansion coefficients between those of GE180

Figure 1. A cylindrical shape 3He SEOP cell made of GE180
with 3He gas of 3.4 atm and alkali metals inside. The
shiny metallic spots are a mixture of rubidium andpotassium.

Figure 2. GE180 cells are fabricated at the IMRAM glass workshop of Tohoku University.

MLF Annual Report 2018

Figure 3. A GE180 cell with the string part.

Figure 4. Connection of GE180 and Pyrex tubes.

and Pyrex to reduce the residual stress. The connecting glasses are prepared by mixing GE180 and Pyrex atratios of 7:3 and 5:5 and placed between the two tubes(Fig. 4). The use of these connecting glasses significantly suppresses cell failures.
3. Gas filling
A GE180 cell with the string is thoroughly cleaned
and then connected to a high vacuum system at KEK.
They are baked out until the pressure reaches theminimum. The alkali metals are then evaporated andchased into the GE180 cell using heaters. Finally, the cell
is filled with a small amount of nitrogen gas and 3He gas
through heated getter gas purifiers and sealed off usinga gas torch. For a 3He cell with a gas pressure of 1 atm,the cell is soaked into liquid nitrogen during the tip-off.
Up to 3.6 atm of 3He gas can be filled with liquid nitrogen. The whole gas filling process takes a few weeks.
4. What’s next?
We have been making cylindrical shape 3He cells
using GE180. The next milestones are the enlargementof the cell diameter to expand the usable neutron beam

Neutron Sciencesize, the increase of the pressure resistance to boost thepolarizable neutron energies, and achieving the longest spin relaxation time for the ex-situ applications,where 3He gas is not polarized in the instrument, but apolarized 3He cell is transported from an optical pumping station in a laboratory to the neutron beamline,
which considerably simplifies the 3He NSF apparatus.
Another important demand is the spin analysis of
scattered neutrons. POLANO covers a wide solid angle
for scattered neutron detection, and the same angle
coverage is desired for the spin analysis. A horseshoeshaped or doughnut-shaped 3He cell will cover such awide scattering angle [4, 5] though it is extremely difficult to fabricate.
An alternative direction of the spin-analyzer development can be a double chamber cell. It consists of
two chambers connected together with a gas transfer
tube; one chamber is for the optical pumping, and theother for the NSF. A 3He gas is polarized in the opticalpumping chamber, and the polarized 3He gas diffuses
into the NSF chamber. The advantage of using a double
chamber cell is that the NSF part can be separated fromthe hot optical pumping chamber, yet the polarizationof 3He is kept constant as the 3He gas is continuously
polarized in the optical pumping chamber.
The fabrication of GE180 aluminosilicate glass cells
is an important key technique in the 3He neutron spin
filter development. Glass cells in various shapes andsizes will be needed for POLANO as well as for otherneutron scattering measurements. The growth of the
3He NSF applications depends strongly on the advancesin glassblowing techniques.
References[1] T. Ino, M. Ohkawara, K. Ohoyama, T. Yokoo, S. Itoh,Y. Nambu, M. Fujita, H. Kira, H. Hayashida, K. Hiroi, K.
Sakai, T. Oku, and K Kakurai, J. Phys.: Conf. Ser. 862
012011 (2017).
[2] T. R. Gentile, P. J. Nacher, B. Saam, and T. G. Walker,
Rev. Mod. Phys. 89, 045004 (2017).
[3] Y. Masuda, T. Ino, V. R. Skoy, and G. L. Jones, Appl.
Phys. Lett. 87, 053506 (2005).
[4] W. C. Chen et al., J. Phys.: Conf. Ser. 746, 012016(2016).
[5] E. Babcock et al., AIP Conf. Proc. 1969, 050005 (2018).

T. Ino1,2, T. Kudo3, Y. Ikeda4, Y. Ohkawara4, M. Fujita4, T. Yokoo1,2, S. Itoh1,2, and N. Kaneko1,2
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3Institute ofMultidisciplinary Research for Advanced Materials, Tohoku University; 4Institute for Materials Research, Tohoku University

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MLF Annual Report 2018

Magnetic Devices and Environment for Polarization
Experiment on POLANO
1. Introduction
Although the polarized neutron spectrometer,
POLANO, is still under commissioning, a part of the user
program was opened for public use with unpolarized
neutron experiments. POLANO is a chopper type spectrometer originally designed with polarization analysis capability [1–5]. Our primary motive for designing POLANO
is to achieve higher-energy polarization analysis of inelastic scattering beyond a reactor-based neutron source.
A wide momentum and energy region is necessary forphysics in multiple degrees of freedom. Our final goal isto realize polarization experiments up to 100 meV of thetransfer energy and around 10 Å1 in momentum space.
The total polarization system on POLANO is now under development, specifically, the development of a spin
exchange optical pumping (SEOP) spin filter used for apolarizer, and a magnetic field system. Both are now inthe process of off-line testing. The magnetic field system
involves magnetic guide fields for maintaining spin polarization, Helmholtz coil system for applying a magnetic field
on a sample, and analyzer mirror. Last year, we reported
on the newly developed cooling system for the Helmholtz
coil system [6]. In this report, we present the follow-up
magnetic field measurement test results of the system.
2. Magnetic field system
The magnetic field system being installed in the
beam line of POLANO is combined with several magnetic devices such as, permanent magnets before the Fermi
chopper, a solenoid coil in the SEOP system, a verticalguide field, Helmholtz coil system, permanent guidefield after the sample, and a magnetic yoke of analyzer
mirror. The Helmholtz coil system is composed of threemagnetic coils for applying horizontal magnetic fields
and a pair of coils for applying vertical magnetic fields.
Since the three horizontal magnetic coils are positioned
triangularly in the horizontal plane, applying magnetic
field can be controlled by tuning the current of each coil.
We conducted the magnetic field measurement
tests with a three-dimensional (3D) probe in order tocheck accurately the applied magnetic field on the sample. The system will be used in a large vacuum chamberof POLANO, precisely controlling the magnetic field bychanging the electric current of the Helmholtz coils.
The test probe with a mechanical translation system
to measure the magnetic field at entire positions in the118

coils was developed as shown in Fig. 1.
By tuning the current ratio, the magnetic field direction can be controlled three-dimensionally in the rangeof 50 Gauss. Figure 2 shows the results of measured
magnetic moments (dotted signals) at various positions
from the sample (x  0). Also, the optimized alignmentsof the magnetic-field devices were evaluated using thefinite elements method software, FEMTET, shown bylines in the figure. Figure 2(a) represents scattering angle
dependence of the magnetic moments in the horizontal
plane, applied to the vertical field. Position 0 in the x-axis
corresponds to the sample position. The calculation by
FEMTET can almost reproduce the measured results, except for deviations at large x. Near the sample positionx  0, where near the sample, the magnetic field is fromthe Helmholtz coil only. The dip in between x  30 to 40,
corresponds to the gap of the Helmholtz coil and the fanshaped guide magnet (FSM). At x  55 cm, the position of
the FSM makes a large field again. In Fig. 2(b), measured
and calculated results of the vertical height dependence
are depicted in the same way. Also, the electrical current
dependences are plotted in Fig. 2(c). The reason why wehave small differences between measured and calculated data is currently unknown. However, the discrepancy of about 5 Gauss cannot be a serious problem forthe guide field. Figure 3 is a horizontal field result plotted similarly to the vertical. In this measurement, there
are some differences between calculated and measured
results at the Helmholtz and FSM position. Again, the differences do not much affect neutron spin polarization.

Figure 1. Newly developed test probe flange. The probe
can be translated by adjusting the slide and rotation mechanism. Radial: from sample position
to 600 mm, rotation angle: from beam center to
120 degrees, height: from beam center to ±30 mm.

MLF Annual Report 2018

50

50

(a)

50

(b)

Vertical Magnet Test

40

'B̲V(8A,-20,0)''B̲V(8A,0,0)'30'B̲V(8A,20,0)''B̲V(8A,40,0)''B̲V(8A,60,0)''B̲V(8A,120,0)''Bcal̲V(8A,-20,0)'20

30'B̲V(8A,0,0)''Bcal̲V(8A,0,0)'20'Bcal̲V(8A,0,0)''Bcal̲V(8A,120,0)''Bcal̲V(8A,60,0)''B̲V(8A,0,30)''Bcal̲V(8A,0,30)''B̲V(1A,0,0)''B̲V(4A,0,0)''Bcal̲V(8A,0,0)''Bcal̲V(4A,0,0)''Bcal̲V(1A,0,0)'

30

20

10
10

'B̲V(8A,0,0)''B̲V(8A,0,-30)''Bcal̲V(8A,0,-30)''Bcal̲V(8A,40,0)''Bcal̲V(8A,20,0)'10
0Vertical Magnet Test
Current dependence of the vertical ﬁeld

40

magnetic ﬂux density [Gauss]magnetic ﬂux density [Gauss]magnetic ﬂux density [Gauss](c)

Vertical Magnet Test
Height dependence of the vertical ﬁeld

Scattering angle dependence of the vertical ﬁeld

40

Neutron Science

20

30

40

50

10
0

60

10

20

30

40

50

60

0

10

20

position [cm]position [cm]

30

40

50

60

position [cm]Figure 2. (a) Scattering angle dependence (current: 8 A, scattering angle: −20 to +120 deg., height: beam center).
(b) Height dependence (current: 8 A, scattering angle: 0 deg., height: −30, 0, 30 mm). (c) Current dependence (coil current:1, 4, and 8 A, scattering angle: 0 deg., height: 0 mm)
50

50

(a)

50

(b)

Horizontal-1 Magnet Test
Scattering angle dependence of H1 ﬁeld

40

(c)

Horizontal-1 Magnet Test
Beam height dependence of H1 ﬁeld

40

Horizontal-1 Magnet Test
Current dependence of H1 ﬁeld

40

'B̲H1(10A,0,0)''Bcal̲H1(10A,60,0)'30'B̲H1(10A,60,0)''Bcal̲H1(10A,120,0)''B̲H1(10A,120,0)'20

10'Bcal̲H1(10A,0,0)'magnetic ﬂux density [Gauss]magnetic ﬂux density [Gauss]magnetic ﬂux density [Gauss]'Bcal̲H1(10A,0,0)''B̲H1(10A,0,0)'30'Bcal̲H1(10A,0,30)''B̲H1(10A,0,+3)''Bcal̲H1(10A,0,-30)'

20'B̲H1(10A,0,-3)'

10

0
10

20

30

40

50

60

'B̲H1(10A,0,0)''Bcal̲H1(1A,0,0)''B̲H1(1A,0,0)'
20

10

0
0

'Bcal̲H1(10A,0,0)'
30

0
0

10

20

position [cm]30

40

position [cm]

50

60

0

10

20

30

40

50

60

position [cm]Figure 3. (a) Scattering angle dependence (current: 10 A, scattering angle: 0 to 120 deg., height: beam center).
(b) Height dependence (current: 10 A, scattering angle: 0 deg., height: −30, 0, +30 mm). (c) Current dependence (coil current: 1 and10 A, scattering angle: 0 deg., height: 0 mm)

Through this series of tests, we concluded that thecalculation using FEMTET can evaluate with high precision the magnetic field with POLANO magnetic condition.
3. Future installation into beam line
Based on this test, we can control applied magnetic
field by YUI device control program. Now, the system isunder safety assessment by MLF. The whole system will
be eventually installed in the beam line, and the polarization commissioning will start soon thereafter.
References[1] T. Yokoo, K. Ohoyama, 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, M. Takeda, K. Kaneko, M. Hino, S. Muto, J.
Phys. Soc. Jpn. 82 (2013) SA035.
[2] 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, S. Choi, J. Phys. Soc. Jpn. 82, (2013) SA036.
[3] T. Yokoo, K. Ohoyama, S. Itoh, J. Suzuki, M. Nanbu, N.
Kaneko, K. Iwasa, T.J. Sato, H. Kimura, M. Ohkawara,
Journal of Physics Conf. Series 502 (2014) 012046.
[4] T. Yokoo, K. Ohoyama, S. Itoh, K. Iwasa, N. Kaneko,
J. Suzuki, M. Ohkawara, K. Aizawa, S. Tasaki, T.
Ino, K. Taketani, S. Ishimoto, M. Takeda, T. Oku, H.
Kira, K. Hayashi, H. Kimura, T. J. Sato, EPJ Web ofConferences 83 (2015) 03018.
[5] T. Yokoo, S. Itoh, N. Kaneko, M. Fujita, T. Ino, M.
Ohkawara, K. Ohoyama, M. Sakaguchi, AIP conference proceedings 1969 (2018) 050001.
[6] M.Ohkawara et al. MLF annual report 2017,p.120–121.

N. Kaneko1,2, T. Yokoo1,2, Y. Ikeda3, M. Ohkawara3, K. Hayashi2, S. Itoh1,2, and M. Fujita3
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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MLF Annual Report 2018

Sample Environment at MLF
1. Introduction
The sample environment (SE) team operates thebeamline (BL)-common SE equipment, prepares and develops new SE equipment, and aids the users in operating the equipment. The SE team consists of 17 members:
8 from JAEA, 1 from KEK, 6 from CROSS and 2 from an
outsourcing company, and is divided into sub-teams ofcryogenics and magnets, high temperature, soft-matter,
pulsed magnet, light irradiation, 3He spin filter, and highpressure. The status and activities of the SE team in
JFY2018 are summarized in this report.
2. Cryogenics and magnets
We have supported users’ experiments using theSE equipment that is commonly used at several beamlines: the superconducting magnet was operated for 16
experiments, the 3He cryostat for 16 experiments andthe dilution refrigerator (DR) insert for seven experiments, including instrument proposals. The 4He cryostat
fabricated by ICEoxford had been under repair due toserious leakages found in January 2018. The cryostat
was returned to our facility after finishing the repair in
March 2019, and we confirmed that all the problems
were solved. Note that another 4He cryostat fabricatedby Suzuki Shokan Co., Ltd. was introduced for users’
experiments twice when the cryostat by ICEoxford was
not available.
3. High temperature equipment
We have two furnaces: a niobium furnace for inelastic and quasi-elastic neutron scattering measurements,
and a furnace for small-angle neutron scattering (SANS)
measurements.
In JFY2018, the niobium furnace was used for two
users’ experiments on BL14 and BL18. On BL21, we measured the background level from the furnace, and foundthat it was acceptable for experiments.
We have upgraded the SANS furnace, installing a
new heater, which contains B4C shielding blocks and cancover both a small-angle detector bank and a middleangle detector bank. From a test measurement, we foundout that the background level was quite small.
4. A pulsed magnet system
In the last fiscal year, we have already developed
a prototype compact and transportable pulsed magnet system for high magnetic fields of up to 30 Teslausing for the commercial liquid helium (LHe)-cooled
120

cryostat, named ‘Orange-cryostat’, with a 70 mm bore
(AS Scientific Products Ltd.). Although a system using cryostats can generally achieve low temperatures (i.e., below
2 K), handling LHe is relatively difficult and inconvenient.
Therefore, in this fiscal year, we are developing a new
insert and a coil using a Gifford-McMahon (GM) refrigerator instead of cryostats. Even users who are not accustomed to LHe can use the pulsed magnet system, thus
improving both convenience and practicality. Figure 1
shows the appearance of the pulsed magnet system,
the insert and the GM refrigerator (HE-05, ULVAC, Inc.).
Neutron scattering experiments using this system were
tested and demonstrated at BL10. An example of an
output pulsed current waveform of the coil is shown in
Fig. 2. The current value at the peak is 3.6 kA at 29.2 Tesla.
In this experiment, the automatic repetitive operation ofthis system was also confirmed to be successful.

Figure 1. The pulsed magnet system.

Figure 2. Example of an output pulsed current waveform.

MLF Annual Report 2018

5. Light irradiation
The mercury lamp light source of the MLF SE common equipment (REX-250, Asahi spectra) was used in
the neutron reflectivity experiment for the first time. The
light shutter can be controlled from the operation cabin
under the device control and data acquisition system tomake possible subsequent automatic measurements
under different conditions.
6. 3He spin filter
We have been developing a spin-exchange opticalpumping (SEOP) based polarized 3He neutron spin filter(3He-NSF) for efficient utilization of pulsed neutrons at
J-PARC.
In JFY2018, we have completed the assembly of a
3
He gas filling station with a vacuum system to fill 3He gas
and alkali metals of Rb and K for the hybrid spin filter cells(Fig. 3). We were able to achieve vacuum pressure lower
than 1  106 Pa within the filling station after baking
at 250°C for stainless parts and 450°C for glass parts foralmost a week. Such a level of low pressure is considered
to be necessary to fabricate high-quality spin filter cells.
We have also developed and introduced an electron
paramagnetic resonance (EPR) and frequency sweep
NMR into our 3He-NSF system to monitor the polarization
degree of the 3He nuclear spin.

Figure 3. The assembled 3He gas filling station with a vacuum
system.

7. High pressure
We have constructed a low-temperature and highpressure (LTHP) system based on the one developed by

Neutron Science

Klotz et al. [1]. The system consists of a Paris-Edinburgh(P-E) cell (VX-5) suspended from the vacuum flange
equipped with a rotation goniometer and a GM refrigerator. Feasibility tests demonstrated pressure generationof 20 GPa at room temperature. Also, we succeeded incooling to 5 K in the low-temperature generation test.
When the P-E cell is precooled with liquid nitrogen, thecooling time to 5 K from room temperature is about
6.5 hours. Until 2017, we used a manual hand pump topressurize the pressure transmission medium, but it wasdifficult to control the pressure for prolonged measurements. We newly installed an automatic pressure pump
(Teledyne ISCO, 30D syringe pump) for precise controlof the pressure. In JFY2018, we carried out an inelastic
scattering experiment at BL01 using this system.
8. Soft matter tensile testing machine
We newly installed the tensile testing machine witha humidity control unit (Fig. 4). The maximum length ofstroke is 100 mm, the load range from 100 N to 1 kN canbe measured, and the relative humidity in the sample
chamber can be changed from 0% to 85%RH. In JFY2018,
we supported the research on ion exchange membranes
using in-situ small-angle neutron scattering experimentat BL15 with this equipment.

Figure 4. Tensile testing machine equipped with humidity
control unit.

Reference[1] S. Klotz et al, High Press. Res., 36, 73 (2016).

M. Watanabe1, T. Oku1, R. Takahashi1, Y. Su1, T. Okudaira1, T. Ino1,2, S. Ohira-Kawamura1,2, S. Takata1,2, K. Sakai1,3, M. Ishikado4, K.
Ohuchi4, H. Arima4, T. Morikawa4, S. Zhang4, Y. Sakaguchi4, Y. Yamauchi5, M. Nakamura5, and K. Aizawa1
1
Technology Development Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science Section, Materials and Life Science
Division, J-PARC Center; 3Neutron Source Section, Materials and Life Science Division, J-PARC Center; 4Neutron Science and Technology
Center, CROSS; 5Nippon Advanced Technology co.

121Neutron Science

MLF Annual Report 2018

MLF Advanced Computational Environment
1. Introduction
The requirements of the instrument scientists andusers to the infrastructure of the MLF computational
environment include the following:• Management of large volumes of data generated
in MLF:¾ Making it possible to manage reliably measurement data that will increase dramatically as
the proton beam power increases.
¾ As the analysis becomes more intermediate,
data and result data (secondary data) generated during the analysis may become very large,
it is necessary to access users’ data quickly andeasily under the authorized access.
¾ Business continuity plan (BCP) in case of adisaster.
• Support for advanced data analysis of the newmeasurement methods developed in MLF, suchas the Multi-Ei measurement, 4D single crystal
measurement, and stroboscopic measurement.
To satisfy these requests, the MLF computing group
started to develop the infrastructure from FY2012. The
construction of the infrastructure, called MLF Advanced

Computational Environment (MLF-ACE), began in
FY2017. In this article, we cover the details of the MLFACE installed in FY2017 – 2018.
2. Solution
The solution for the requests mentioned aboveis the MLF-ACE, composed of the following four
components:• Broadband and redundant network• Large scale parallel access storage• File sharing system• Analysis factory
Figure 1 is the schematic view of the MLF-ACE. In
FY2017 – 2018, the broadband and high availability
network, a part of the large-scale parallel access storage
and the file sharing system have been installed. It is a
fault tolerant system. The specification of these components is shown in Table 1. In compliance with the BCP,
the components in the J-PARC Research Building (JRB)
are installed on the second floor.
The network includes two layers. One is the main
layer and the other is a branch. The main layer is the
network between the four core switches at JRB and the

Figure 1. The schematic view of the MLF-ACE.

Table 1. Specifications of the MLF-ACE introduced in FY2017 – 18.

Component

122

Specifications

Network

Instruments (BL switches27) – Aggregation switches4 at MLF: 10 Gbps/BL
Aggregation switches4 – Core switches4 at JRB: 40 Gbps2
Core switch – File sharing system: 10 Gbps4

Storage

200 TB2 (Volume: 100 TB4)
Fiber channel switch2
File sharing system: Metadata2, Gateway
File sharing system – Storage: 16 Gbps4 (Fiber Channel)

Monitor

Network traffic monitoring server, Traffic visualization software

MLF Annual Report 2018

four aggregation switches at MLF. The branch layer connects the aggregation switches and 27 BL switches at
each instrument including 23 neutron beamlines andfour muon beamlines. The network bandwidth is broadband, which is that the main layer is double 40 Gbps andthe branch layer is 10 Gbps. All network lines are wiredwith optical fibers except in the server room in JRB. The
main layer has high availability, every core switch, aggregation switch and wire is paralleled. The paths between the switches are a cross-over connection. So,
if a single failure occurs, the paths are automaticallyswitched and the network communication continues.
All switches have duplicated power supply units.
The storage consists of two units to balance theload. One unit will store the data generated with the
instruments at the MLF first experimental hall, the otherwill be stored at the second experimental hall in parallel. Currently, one storage unit consists of two 100 TB
data volumes. The storage is also redundant. In each
unit, there are duplicated storage processor and Raid6
disk volumes distributed in six enclosures. The power
supply units of each enclosure are also duplicated.
The file sharing system is not maintained by a software service such as NFS and something similar, but by
a dedicated appliance. Currently, the appliance consists of two metadata servers and one gateway server.
As the data traffic amount increases, we will be able
to add gateway servers. They are connected with thestorage via Fiber Channel switches. The bandwidth is

Neutron Science

16 Gbps4 per Fiber Channel. The connection between
the core switches and the file sharing system is 40 Gbps
Ethernet. All connections are also redundant.
In addition, a network traffic monitoring system has
been installed. The system consists of a network trafficmonitoring server and a visualization workstation withtraffic visualization software. The operator can watch all
network traffic in the MLF-ACE in real time.
3. Current status
In the instruments introduced at the MLF-ACE, it
is possible to reduce the time allocated to data management. For example, the instrument staff currently
handle the data backup for each instrument. After the
MLF-ACE is installed, the data generated from the DAQ
system will be stored directly in the available high-capacity storage of the MLF-ACE. Thus, because the instrument staff do not need to manage the data, they
will concentrate on other tasks, such as data analysis.
4. Future plans
The DAQ system in several instruments and thestorage of the MLF-ACE will be connected in FY2019.
The storage will be expanded, and the analysis factory
will be introduced as soon as possible. In the analysis factory Live Data Reduction will be performed. In
the future, the so-called “data mining” and “Materials
Informatics” methods will be applied to the data stored
in the MLF-ACE.

T. Nakatani
Technology Development Section, Materials and Life Science Division, J-PARC Center

123

Neutron Science

MLF Annual Report 2018

A 200-Micron Spatial Resolution Scintillation Detector
for Time-of-Flight Neutron Diffraction Imaging
1. Introduction
Neutron diffraction imaging is a powerful technique to evaluate spatial distribution within materials,
such as texture, grain orientation, and gain size. Witha combination of a pulsed neutron source energy-selective neutron images can be measured, providing uswith spectroscopic information about the transmission
or diffraction spectra. More precise diffraction images
can be obtained by using well defined, high-intensity
pulsed neutron beam in the J-PARC MLF.
Our purpose is to develop a high-resolution, twodimensional neutron detector for time-of-flight diffraction imaging. Although superior high-resolution
detectors have been developed, such as n-MCP [1],they are not always available or do not suit perfectly
our requirements. We introduce here our solution toprovide such detectors with a scintillator / wavelength
shifting (WLS) fiber detector technology.
2. A scintillator / WLS fiber detector
The scintillator / WLS fiber detector has a great flexibility in designing the detector head. This technique
has proven to work well to develop a position-sensitive
neutron detector [2, 3]. The detector specifications,such as pixel size and spatial resolution, can be designed by selecting properly tuned detector components. A two-dimensional neutron detector is requiredin our experiment with a spatial resolution of about
100 m and with a neutron-sensitive area of more than
20  20 mm. In order to meet these requirements, theneutron-detecting head was made by using WLS fibers with a diameter of 100 m. These fibers are speciallymanufactured for this purpose. Figure 1 shows a photograph of the prototype detector. In order to make fiber
arrays, the WLS fibers were aligned in flat without air
gap between them. Two of these fiber arrays were produced and each array contained 224 fibers. They werearranged diagonally in contact with each other, making fiber channels for x and y directions. On top of thecrossed fiber arrays a single 6Li:ZnS scintillator screen
was implemented. The scintillator screen was grinded
down to 0.17 mm to lower the light spread within the
scintillator. It ensures a high spatial resolution of thedetector. The detector specifications are summarizedin Table 1.

124

(a)

(b)

WLS fibers

Scintillator
24 × 24 mm

Figure 1. (a) Photograph of the 200-μm spatial resolution
scintillation detector. (b) Inside view of the neutron
detecting head.
Table 1. Detector specifications.

Neutron-sensitive area
Pixel size
Channel number
No. of pixel
Photomultipliers
Physical size
WeightPower dissipation

:
:
:
:
:
:
:
:

24 × 24 mm
107 × 107 μm
224 × 2 ch
50176
MaPMT (64 ch) × 8
40w × 45d × 30h cm
25 kg
135 W

3. Detector performances
The detector performances were evaluated by using a pulsed neutron beam in the BL10 of the J-PARC
MLF. In order to check the image reconstruction, thedetector measured the neutron beam with a Cd cut-out
mask placed on the detector window. The detector was
positioned at the distance of 13 m from the moderator. Figure 2 shows (a) a photograph of the Cd mask and(b) the measured transmission image. Only the limitedarea shown by the dot line in (a) was irradiated withneutrons. The detector reproduced the shape of cutout
letter well, confirming the proper positioning schemeof the detector system.
A spatial resolution of the detector was evaluatedby measuring the beam-edge of the collimated beam.
A Cd mask covered the part of the neutron-sensitive
area as the mask edge was placed normal to the WLS
fibers. The measured transmission profiles were thenanalyzed by fitting with a linear-spread function. The
spatial resolutions are represented in full width at half
maximum (FWHM). Figure 3 shows the measured spatial resolution in (a) x-direction and (b) y-direction forMLF Annual Report 2018(a)

Neutron Science

(b)

5 mm

Spatial resolution (mm)0.4

Spatial resolution (mm)Figure 2. (a) Photograph of the Cd mask. Only the area withthe dot line was irradiated with neutrons. (b) the
measured transmission neutron image with the
mask.

0.4

5 mm

Figure 4. Example of neutron diffraction images measured
with the prototype detector [5].

x-direction
0.3

diffraction images measured in the BL10 of the J-PARC
MLF. Details of the experiments can be found in [5]. The
coarse-grained electromagnetic steel plate was set as asample at the distance of 13.4 m from the pulsed neutron source. The detector was located close to the sample at a distance of 7 cm from the sample at 90°. Manydiffraction spots were traced clearly in the measured
images, confirming the feasibility of the detector.

0.2
0.1
0.0

y-direction
0.3
0.2
0.1
0.0

0

1

2

3

4

5

6

7

8

9

10 11 12 13

Fiber position

Figure 3. Spatial resolution (FWHM) of the detector [4].

neighboring 12 points. The detector exhibited spatial
resolutions of 0.200.06 mm and 0.160.06 mm in average for x and y directions, respectively.
The detection efficiency of the detector was evaluated to be 7% for thermal neutrons (1.8 Å). This value
was about half of the neutron absorption rate in the
scintillator screen. The trigger rate could be increased
by lowering the threshold of discriminator electronics with a cost for gamma-ray sensitivity. Under thisoperational condition, the 60Co gamma-ray sensitivity
reached 1  106 for 1.17 and 1.33 MeV gamma rays. This
was acceptable for our demonstrative experiment.
Figure 4 shows one of the time-of-flight neutron

4. Conclusions and future works
The high-resolution neutron detector was developed by using the scintillator / WLS fiber detector
technology. The developed detector was implemented successfully into the demonstrative experiment for
time-of-flight neutron diffraction imaging in the J-PARC
MLF. In the future, the detection efficiency will be improved by adjusting the 6Li content in the scintillator
and/or by equipping multiple scintillator / WLS detecting heads.
References[1] A. S. Tremsin, et al., Nucl. Instrum. & Meth. A 787(2015) 20.
[2] T. Nakamura, et al., Nucl. Instrum. & Meth. A 737(2014) 176.
[3] T. Kawasaki, et al., Nucl. Instrum. & Meth. A 735(2014) 444.
[4] T. Nakamura, et al., Conference record, 2018 IEEE
Nuclear Science and Medical Imaging Conference.
[5] T. Kawasaki, et al., Physica B: Condensed Matter 551(2018) 460.

T. Nakamura1, K. Toh1, T. Kawasaki2, and K. Sakasai1
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science Section, Materials and Life Science
Division, J-PARC Center
1125Muon ScienceMuon Science

MLF Annual Report 2018

Status of J-PARC MUSE: Overview
Muon Science Division is responsible for the interuniversity user program and the operation, maintenance and construction of the muon beamlines; theD-Line, S-Line, U-Line, and H-Line as well as the muonsource at MLF.
1. D-line
At the D-Line, variety of new scientific activities suchas archeology, industrial application, and fundamental physics by using the world’s most intense negativeand positive muon beam have been performed, withbudgetary support from the collaborative research ofInter-University Research Institute Corporation and by“Toward new frontiers: Encounter and synergy of stateof-the-art astronomical detectors and exotic quantum beams” (Grant-in-Aid for Scientific Research on
Innovative Areas from Ministry of Education, Culture,
Sports, Science and Technology). The high-intensity
negative muon (P) beam and counting system has
drastically increased the data acquisition rate for PSR
to over 2u104 events/s (72 M events/hr), allowing thecompletion of a PSR experiment within an acceptable
time. For example, the first observation with PSR of
the nuclear magnetic field in MgH2 is featured in the
research highlights of this volume.
2. S-line
At the S-Line, the stable operation at the S1 area
continues. Thirty-four experiment proposals in 2018

have been carried out, including one urgent proposal
and three P-type proposals. During the 1-MW test operation in July 2018, the integrity of the PSR data acquisition system and the beamline equipment at the
S-line was confirmed. It was successfully demonstrated
that the PSR spectrometer, ARTEMIS, can handle a dataacquisition rate as high as 370 million events per hour.
3. U-line
At the U-line, the depth profile experiments using decelerated ultra-slow muons were successfully
performed in a silver film on a silicon dioxide plate inJune 2018. The double permalloy magnetic shield forthe tungsten target was installed in September 2018
for suppressing muon-spin depolarization by stray fieldfrom the beamline magnets. A muon reacceleration experiment using an induction accelerator will soon be
conducted at the U1B area.
4. H-line
At the H-Line, electric power of about 5 MW is necessary to operate all components of the H-line, so, a
new electric power sub-station is being constructed in
the northeast side of MLF. In FY2018, the platform of
the sub-station was completed and high voltage cables
were laid. The electric construction, including cabling
work from the new sub-station to the experimental hallof the MLF, is planned for FY2019.

Y. Miyake1,2, S. Takeshita1,2, A. Koda1,2,Y. Ikedo1,2, T. Yamazaki1,2, K. Shimomura1,2 , N. Kawamura1,2, P. Strasser1,2, Y. Oishi1,2,
Y. Nagatani1,2, H. Fujimori1,2, S. Makimura1,2, Y. Kobayashi1,2, J. Nakamura1,2, T. Adachi1,2, M. Tampo1,2, W. Higemoto2,3, and T. U. Ito2,3
1
Institute of Materials Structure Science, KEK; 2Muon Science Section, Materials and Life Science Division, J-PARC Center; 3Muon Science
Section, Materials and Life Science Division, J-PARC Center

128

MLF Annual Report 2018

Muon Science

Report on the Trouble of the Rotation System and the
Taken Measures
1. Introduction
A pulsed muon beam with unprecedented intensity will be generated by a 3 GeV 333 PA proton beam
on a muon target made of 20 mm thick isotropic graphite at J-PARC MLF MUSE (Muon Science Establishment).
The energy deposited by a 1 MW proton beam is estimated to be 3.9 kW in the muon target. The ﬁrst muon
beam was successfully produced on September 26,
2008. Gradually upgrading the beam intensity, a continuous 300 kW proton beam has been operated bya fixed target method without replacements till June
2014. However, the proton-irradiation damage to thegraphite caused by the 1-MW proton beam operation, will reduce the lifetime of the fixed target to lessthan a year. To extend the lifetime, a muon rotatingtarget, in which the radiation damage is distributed toa wider area, had been developed. The muon rotatingtarget was installed in September 2014. The rotatingtarget has been successfully used for five years without replacement. Since 2018, a continuous and stable
500-kW proton beam has been operated successfully.
The accumulated operational period and the number of revolutions have reached 13500 hours and 12.5
million, respectively, by March 2019. Furthermore, on
July 3, 2018, a 1-MW beam operation for 1 hour (beampower, 935 kW: 1 MW equivalent for one pulse) was
successfully achieved. Meanwhile, a failure on the rotation system, which could potentially lead to a loss ofthe transmission, was discovered during the long shutdown in September 2018. At present, the operation of
the rotating target is being monitored carefully andmeasures have been taken to prevent the loss of thetransmission. In this report, the trouble of the rotation
system and the measures taken at J-PARC MLF MUSE
will be covered.
2. Failure on the rotation system
When the rotation feedthrough between a vacuum
and air was replaced as part of the regular maintenancein September 2018, the damage on the flexible coupling that connects the feedthrough and the rotation
shaft was discovered. Though the coupling had survived in spite of the damage, it broke into pieces completely during the replacement process. We recognizedthat the damage originated from the drawing instructions for the machining of the coupling. Inappropriate

Figure 1. Pictures of the rotating target assembly (right), thereplacement of the vacuum feedthrough with theglove box (left-up), and the broken flexible coupling (left-down).

couplings were employed on the two positions of therotation system. Figure 1 shows pictures of the rotatingtarget assembly (right), the replacement of the vacuum
feedthrough with the glove box (left-up), and the broken flexible coupling (left-down). While the broken coupling was replaced immediately with the appropriate
one, it was difficult to replace the other one before therestart of the beam operation because of its hard accessibility, the high residual radiation dose, and the highcontamination of tritium. Consequently, we decided
to keep using the inappropriate coupling with carefulmonitoring and planning for measures to take in caseof loss of the transmission.
3. Analysis of the rotation stop
The most reliable way of detecting the rotation
stop during the proton beam operation is by observing the increment of the torque of the rotation motor.
129

Muon Science

MLF Annual Report 2018

When the coupling breaks down, the detection might
not work as expected. Therefore, the variations of thetemperature and the subsequent thermal stress were
carefully evaluated through a finite element method,
ANSYS.
The graphite itself is divided into three pieces torelease thermal stress caused by the temperature difference on the graphite. The divided three pieces areheld together as a target wheel by the centrifugal-force
ring made of Inconel 600 (Daido Special Metal Co. LTD.).
The weight of the target wheel is 3 kg, and its temperature reaches 930 K. The target wheel is supportedby the rigid wheel support through the nine flat bars
made of Inconel 600. The cutting section of the flatbar is rectangular of 1 mm by 10 mm, and the lengthof the rectangle is 35 mm. The rectangle is located inparallel with the circumferential direction of the target
wheel to release the thermal stress originating fromthe large temperature difference between the target
wheel and the wheel support, as well as to support theweight of the target wheel. Figure 2 shows a picture of

Figure 2. Pictures of the rotating target.

the rotating target. To validate the effect of the rotation stop, the maximum temperature of the graphite,
the thermal stress on the graphite, and the thermal
stress on the flat bar are evaluated. To save time for thesimulation, the simplified 3-dimensional model of thegraphite wheel is used for FEM code since the results
are similar to those of the full model. The thermal stresson the flat bar is evaluated by a theoretical calculation
with a double supported beam model, where the rotation is restricted on the both ends. The criteria of the
maximum temperature of the graphite, the thermal
stress on the graphite, and the thermal stress on the flatbar are 2300 K, 25 MPa, and 200 MPa, respectively.
As a result of the simulations, it was confirmedthat the allowable beam intensity without rotation was
500 kW. When the beam intensity exceeds 500 kW without rotation, the graphite will probably crack and theflat bar will be plasticly deformed. However, even if thetemperature of the graphite reaches 2300 K, the evaporation rate of the graphite is still low enough (1.4 Pm/hour). Furthermore, the used rotating target can be
replaced with a new one, because the aperture of thetarget chamber is large enough to extract the rotatingtarget, even if the flat bars are plastically deformed. On
the other hand, the radioactive gases, including tritium,
are produced and stored in the graphite during thebeam operation. The radioactive gases from the graphite at high temperature should be taken into account.
4. Restart of the beam operation
Because the results showed that 500 kW powerof the beam operation was acceptable, we decided tokeep using the current rotating target with the inappropriate couplings. To detect the rotation stop immediately, the sensitivity of the machine protection system,
such as the quadrupole mass spectrometer, the torquemonitor of the rotation system, and the temperature
measurement has been improved [1]. To avoid the release of the emitted radioactive gases to the outside of
the facility via the vacuum pumping system, a buffer

Table 1. Results of the analyses under the conditions of 500 kW and 1000 kW with rotation (W/R) and the conditions of 500 kW,
700 kW, and 1000 kW without rotation (W/O/R).

Max. temp. of Graphite (G.) (K)Temp. difference on G. (K)Equivalent stress on G. (MPa)Temp. of CF ring
Equivalent stress on flat bar

130

Criteria 500 kW W/R 1000 kW W/R 500 kW W/O/R 700 kW W/O/R 1000 kW W/O/R
2300
740
880
1690
1990
2390
30
50
950
1220
1600
25
0.7
1.1
22
29
38
450
910
1000
200
80
180
240
-

MLF Annual Report 2018

tank was employed to keep the pumped gas tentatively
until confirming its activity to be low enough [2]. The rotating target had retreated to the escape position from
October 20 to November 6 to validate the new vacuum
pumping system and the buffer tank. At present, a 500kW proton beam has been stably operated with therotating target. In the long shutdown of 2019, the replacement of the inappropriate coupling or the replacement of the entire rotating target assembly is planned.

Muon Science

5. Acknowledgement
I would like to thank to support of the dedicatedstaffs from The NIPPON ADVANCED TECHNOLOGY CO.,LTD (NAT).
References[1] S. Matoba et al., ibid.
[2] N. Kawamura et al., ibid.

S. Makimura1,2, S. Matoba1,2, and N. Kawamura1,2
Institute of Materials Structure Science, KEK; 2Muon Science Section, Materials and Life Science Division, J-PARC Center

1131Muon Science

MLF Annual Report 2018

Negative Muon at D Line – Beamline Commissioning
1. Introduction
The D line, which is a beamline located at MUSE,
MLF, has a long superconducting solenoid and therefore can supply positive and negative decay muons
from several MeV/c to a100 MeV/c in addition to surface
muons. Since the energy of the primary proton beamof MLF is as high as 3 GeV, the generation efficiency ofnegative muons is high. In particular, because the power of the primary proton beam has been incrementally
increased in recent years, the D line now supplies theworld’s highest intensity negative muon beam. Using
the high-intensity negative muons, applications for various experiments such as non-destructive elementary
analysis using muonic X-rays, and negative muon spin
relaxation, are being developed. In this report, we cover
the current status of commissioning the negative muon
beam at D line.
2. Kicker tuning for negative muons
MLF provides double bunch beams with a period of
25 Hz. Each bunch has an FWHM of 100 ns and a bunchinterval of 600 ns. By dividing the double bunch beam
into two single bunches with an electro-magnetic kicker (DKKR1, 2) installed at the branch section, it becomes
possible to supply a single bunch beam simultaneously
in areas D1 and D2.
The branch section consists of two switchyard magnets (DSY1, 2, the so-called bending magnet), two kicker electromagnets (DKKR1, 2), and septum magnets,
which conduct the muon beam toward areas D1 andD2 (DSPTM1, 2) (Fig. 1(a)).

Without kicker excitation, the beam trajectory isslightly bent toward DSPTM2 by DSY1 and 2 and led toarea D2 by the DSPTM2 (Fig. 1(a)). If the kicker is excitedwith an appropriate voltage when the second bunch ofthis beam passes through DKKR1 and 2, only the second
bunch is bent toward the DSPTM1 and then conductedto the area D1 (Fig. 1(b)). Since DKKR is unipolar, the single bunch operation for negative muons requires thatthe kicker be operated to the double bunch beam supplied to the D2 area.
The optimal kicker excitation voltage and excitation
timing depend on the momentum of the muon beam.
The kicker excitation voltage and the excitation timing
were tuned for the negative muon beam of 30 MeV/c.
Regarding excitation timing tuning, we measured by installing scintillation counters in both D1 and D2. Whilechanging the delay of the kicker excitation trigger, wefound the condition that the first bunch was conductedto D2 without any loss and the second bunch was also
conducted to D1 without loss. The kicker excitation
voltage was tuned by measuring the intensity of thenegative muon at D1 with the scintillator while changing the excitation voltage. As a result, an excitation voltage of r27 kV was optimal at 30 MeV/c. The result of
this tuning is shown in Fig. 2. The double bunch beamobserved at D2 without the kicker operation is supplied
as a single bunch beam to D1 and D2 by the kicker operation. Considering that the kicker rating is r40 kV, it
can be expected that a beam of about 40 MeV/c can bekicked.

Figure 1. Schematic view of the branch section with the kicker system and its operation (a) without and (b) with kicker excitation.

132

MLF Annual Report 2018

Muon Science

Figure 2. Muon intensities as a function of time observed by scintillation counter at areas D1 and D2.
(a) Double-bunch structure of the negative muon beam observed at area D2 and (b) Singlebunch structure by exiting DKKR1 and 2 observed at both areas.

3. Separator upgrading
In measurements, such as elementary analysis bymuonic X-rays and muon spin relaxation, contamination of prompt electrons becomes a noise source andmust be filtered as much as possible. For this reason, aDC separator (DSEP, the so-called Wien filter) has been
installed in the D line. The DSEP consists of high-field
electrodes for applying a high electric field, and correction coils for applying correction magnetic field tocorrect the trajectory of the muon bent by the highelectric field, where the direction of the magnetic fieldis orthogonal to the electric field. However, discharge
had frequently happened during the operation, andtherefore the operation voltage of the electric field has
been limited to r170 kV for stable operation. During
the summer maintenance in 2018, the high-voltage
power supply was replaced with a revised new system
so that a higher electric field can be applied, and thisupgrade improves the efficiency of reduction of theprompt electron.
The high-voltage power supply for DSEP had been
located next to area D2 and connected to the electrodes of the DSEP via a high-voltage cable with lengthof approximately 10 m. Since frequent discharge happened in this electrode connection part, the high-voltage power supply was replaced with the one that had
been tested and approved at the U and S line (Fig. 3).
This high-voltage power supply is of the Cockcroft typeand is placed directly above and below the main bodyof the DSEP. The electrodes of the high-voltage power
supply are directly connected to the separator electrodes inside the chamber. As a result, it was possible toapply an electric field of up to r250 kV.
In order to measure the effect of the high electricfield, a stacked pair of scintillation counters were installed in area D2. The intensities of the negative muonsand contaminated electrons in the beam were measured by the counter of the upstream and downstream,
respectively. The upstream scintillator has enoughthickness to stop all muons, so that the downstream
counter observes only the signal of the electrons.
Figure 4 shows the intensities of the negative muons and the electrons as a function of the correction
coil current at DSEP with applied voltages of r170 kV
and r240 kV at 30 MeV/c. From the muon intensity,
the optimal correction coil current was a60 A at an applied voltage of r170 kV, while it increased to a60 A
at r240 kV. As a result, the ratio of the intensity of thecontaminated electrons at r240 kV compared to thatat r170 kV is 13% (87% of electrons are thoroughly filtered). However, due to the failure of the high-voltage
power supply, which happened in February 2019, currently, the applied voltage is limited again to r170 kV.
This power supply will be replaced with a new one during the 2019 summer shutdown.

133Muon Science

MLF Annual Report 2018

Figure 3. Installed Cockroft type high-voltage power supply
on the DC Separator (DSEP).

Figure 4. Intensities of muon and contaminated electron at±240 kV and ±170 kV excitation.

S. Takeshita1,2, P. Strasser1,2, Y. Ikedo1,2, M. Tampo1, S. Doiuchi1, A. Hashimoto1, I. Umegaki3, T. U. Ito4, S. Nishimura1,2, N. Kawamura1,2,
K. Shimomura1,2, and Y. Miyake1,21Institute of Materials Structure Science, KEK; 2Muon Science Section, Materials and Life Science Division, J-PARC Center; 3Toyota Central
Research & Development Laboratories, Inc.; 4Advanced Science Research Center, JAEA

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Development of the Ultra-Slow Muon Beam at the U-line
1. Overview of the U-Line
The Ultra-Slow Muon (USM) beam, which has quite
low kinetic-energy, small beam-size, and small-time distribution, is needed to probe surface and inter- face ofmaterials. In J-PARC, a muon beamline (U-Line) for USM
was constructed and currently is under commissioning [1]. In the U-Line, an intense surface muon beamis transported by superconducting solenoids and incidents to a muon production target. A part of the muons
stopped in the tungsten evaporate as muoniums. A resonant laser ionizes muoniums to produce a USM beam.
Then, the USM beam is accelerated up to 30 keV andis transported to the U1A area or the U1B area. At the
U1A area, the USM beam is provided to a PSR spectrometer on a high voltage stage. To control the penetration
depth to a sample, the kinetic energy of the USM beam
is controlled by the deceleration voltage, which is applied to the stage.
2-1. Improvement of the magnetic shield
Strong stray field from the superconducting solenoids affects the extraction of USM. The magnetic
shielding of the muonium production chamber was improved during the summer shutdown of 2018. A double-layered permalloy shield was installed in between
the muonium chamber and existing iron shields. The
iron shields were also improved as forming triple layers.
The layout of the shield is shown in Fig. 1. The magnetic
field under the shield was calculated and measured.
The results are shown in Fig. 2. The measured fields
agree with the calculated fields within 0.1 mT.

Figure 2. Magnetic field without using correction coil. Fields
in the center of the beamline are shown. Lines areshowing the calculated field with each season’smagnetic shield. Dots are the measured field withthe latest magnetic shield.

2-2. Control of penetration depth
Following the last year’s successful observationof muon-spin-rotation of USM [2], we tested scanningof penetration depth. The test sample was 50 nm Ag
coated SiO2 plate. A schematic of the test is shown in
Fig. 3. According to the deceleration of USM, the asymmetry increased. It means the stopping region of USM
changed from SiO2 to Ag.

Figure 3. Schematics of the penetration-depth controlling
test.

Figure 1. The layout of the magnetic shield calculated andmeasured.

3. The progress of the laser system
Lyman-D laser system has been operated so far bymaking minor upgrades. In order to increase the stability of the output pulse energy, a few major upgrades
were applied to the laser system.

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3-1. Laser system for ultra-slow muon generation
Ultra-slow muons can be generated by resonant
optical ionization of thermal muonium from hot-W foil
target using 122.09 nm coherent light pulse for 1s-2p
excitation and 355 nm coherent light pulse for ionization. The high-energy pulsed coherent Lyman-D light(122.09 nm) source is a very important element for theefficient generation of high-power ultra-slow muons.
The design of the Lyman-D light source is describedin Ref. 1 and schematic of the light source is shown in
Fig. 4. The pulsed Lyman-D is generated by 2-photon
resonant four-wave mixing in krypton gas. The required
2-photon-resonant 212.556 nm and 820 nm pulses are
obtained by nonlinear wavelength conversions of intense 1062.78 nm pulse. The intense 1062.78 nm pulse
is provided from wavelength locked all-solid-state laser
amplifiers with Nd:YGAG ceramics as an efficient gain
mediums. The all-solid-state laser amplifiers and subsequent wavelength converters that were placed in
the temperature-controlled laser room require minimalmonthly adjustment, and have been working stably
for several months. Even if the laser’s operation is very
stable, the problem of the slow intensity suppressionof Lyman-D intensity by Kr-Ar mixture gas degradation
still remains, which was pointed out in the previous
year’s facility report. In order to reduce that effect, themixture is automatically exchanged every 3 hours.
3-2. Improvement of the laser beam’s pointing stability
Since the Lyman-D generation by four-wavemixing requires the spatiotemporal overlapping of
212 nm and 820 nm pulses in the gas cell, laser pointing stability is important. When the temperature in thelaser room rises due to unexpected blackouts, summer
long shutdown and/or thermal condition changing of
flash lamp pumped Nd:YAG laser for 355 nm generation, an irreversible misalignment of the optical passin the laser system appears. A stress transformation ismainly introduced by the difference of thermal expansion coefficient between breadboards and optical table. The laser system was modularized on the 15 mm
thickness aluminum solid breadboards. Three amplifier
modules (Regenerative, intermediate and power amplifier) and wavelength conversion stages (212.556 nm
wavelength converter and 820 nm parametric amplifier) were placed on the optical table made of stemlesssteel. In order to avoid this problem, all optomechanicalcomponents were relocated from breadboards to theoptical table directory during the summer shutdown in
2018. The effect of this is under evaluating in the day by
day operation. In addition, the optical setup displays instability at the height adjustment periscopes matching

Figure 5. Side view of the optical table and optical pass setup.

7

Distributed
feedback laser

Mag. ~10 )1062.78 nm= 1 GHz

50nJ

Regen. amp.

Intermid. amp.

Power amp.

~2 mJ~100 mJ~1 J
Under construction

Nonlinear frequency conversion
2ndHG

4thHG

100 mJ

5thHG

Lyman- generationin Krypton gas cell
4p55p

Tunable Ti:S
laser

OPA
820.649 nm

To ultra-slow muon
generation
122.088 nm

4s24p6

Figure 4. Schematic of the Lyman-α laser system for the Ultra-slow muon generation.

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Muon Science

Figure 6. Variation of beam pointing in the beam diameter of ~4 mm for 212 nm pulses and ~6 mm for 820 nm pulses.

the height with the Kr gas cell and the muon beam line.
In order to reduce the beam pointing instability, theheight of the optical table was padded by just 300 mm.
We measured the beam pointing stability before andafter the changing of the height of optical table by a
CCD camera which placed at Kr gas cell. Figure 6 shows
the variation of shot to shot laser beam center position
for (a) 212 nm pulses and (b) 820 nm pulses, respectively. For both wavelength pulses, the beam pointing
stability was improved by almost 20%. We will continue
to improve the pointing stability to realize stable Ultraslow muon generation.
4. U1B Area
We are developing transmission muon microscopies
at the U1B area. The final goal of the transmission muon
microscopies is visualizing thick object (! 10 Pm) in nanometer resolution. The re-acceleration of the ultra-slow
muon beam provides quantum coherence of the beamand deep penetration through a specimen. Coherent
muon beams can visualize electromagnetic fields in thickspecimens in high resolution. The transmission muon
microscopy will become a unique research method.
4-1. Prototype of the transmission muon microscopy
This year, a prototype of the transmission muon
microscopy is being constructed at the U1B area. The
purpose of the prototype is to obtain a direct proofof the quantum interference of muons, by detecting

diffraction patterns of the ultra-slow muon beam. The
experiment will be the first direct proof of the waveparticle duality beyond the second generation of theStandard Model. A camera-chamber with a 2-dimensional image sensor is installed after the object lens,
including a specimen stage. The prototype employs the
30keV ultra-slow muon without any additional acceleration. We have confirmed that the incoming muons
can be visualized as dot-images by the system.

Figure 7. The prototype of the transmission muon microscopy in the U1B area. The optical devices of the
microscopy are constructed on a surface-plate ofstone. The ultraslow muon beam is coming fromthe right side. An object lens and a specimen-stage
are stored in the silver cylinder. A multi-channel
plate (MCP) and a phosphor plate are installed in
the left chamber. The MCP converts incoming muons into electrons conserving position of muons.
The electrons are converted into lights by the phosphor plate. Amplification of the MCP is enoughhigh for visualizing single muon for naked eyes. The
image on the phosphor is taken by a CCD camera
at the left end.

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Figure 8. Principal part of the induction accelerator. The horizontal white duct is a beam pipe. The duct is passing through 6 induction cores. Each core is madeby finemet material and accelerate particles up to
6 kV. The vertical white tube behind the beam pipe
is a thyratron, which discharges ceramic capacitors(brown and white cells) into the induction cores.

4-2. Induction accelerator for muons
We have constructed an induction accelerator formuons. The main aim of the induction accelerator is toconduct a muon diffraction experiment for different energies of muon-beams. The diffraction pattern should
be shrinking due to the increase of the beam energy.
By accelerating more than 30 keV, we can choose morekinds of specimens for diffraction-experiments due toincreasing its penetration.
The induction accelerator has been constructed andtested in the Tsukuba campus. In the test, we employeda pulse electron beam generated by a photocathode,and a magnetic deflector as an energy spectrometer.
It was confirmed that the accelerator fully works, andit has been transported from the Tukuba campus to
J-PARC/MLF.
References[1] A. D. Pant et al., JPS Conf. Proc. 21 (2018) 011060.
[2] T. Adachi et al., KEK-MSL Progress Report 2017(2018) 13.
[3] N. Saito et. al., Opt. Express 24, 7566–7574 (2016).

T. Adachi1,2, Y. Ikedo1,2, Y. Oishi1,2, Y. Nagatani1,2, and M. Yoshida3
1
Institute of Materials Structure Science, KEK; 2Muon Science Section, Materials and Life Science Division, J-PARC Center; 3Accelerator
Laboratory, KEK

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Development of Sample Environment at the S1 Area
1. Introduction
There is a growing demand for the PSR experiment
at low temperatures below 1 K at MUSE, which leads
to the chronic shortage of beam time for 3He-4He dilution refrigerator (DR) installed to the D1 instrument.
In order to settle this issue, we have commissioned a
new 3He evaporation cryostat, which has certain advantages (e.g., portability, cooling efficiency) against
DR. The cryostat is based on a commercially available
model (Heliox AC-V supplied by Oxford Instrumentsplc), which was customized for passing a muon beamthrough the outer vacuum chamber and related partsaround the sample space (see Fig. 1).

Figure 1. A snapshot of the new 3He evaporation cryostat
placed at the test bench.

2. Cooling performance
The cryostat consists of a 3He insert and a twostage pulse tube cryocooler (PTC) operated by a dedicated compressor (Fig. 2), which allows cryogen-freecooling system. The 3He insert consists of a sorption
pump (sorb), a 3He pot, and a heat switch (HSW). A sample is mounted on the base of the 3He pot for temperature control by thermal conduction. A muon beam isdelivered to the sample in vacuum through a 30-mmI
aluminized mylar window. The 3He condensation is realized by the PTC second stage (a3 K) and an outgassing
sorb, while the cooling is attained by pumping 3He gas
using the sorb cooled via HSW.
An example of cooling-down trend for the sample
temperature is shown in Fig. 3. Apart from the holding
time attained by heater control, it takes 1.5 days to reachthe base temperature (0.3 K) from ambient temperature.

Since the cryostat is not designed for the top-loading
holder, it needs warming up to the room temperature
upon sample exchange (taking ca. 9 hours).
We also examined the influence of eddy current induced by changing magnetic field. Figure 4 (left) shows
the temperature trend at the base temperature, where
the its rise is observed with various ramping rates forchanging a magnetic field in 50 G step. The right side ofFig. 4 shows the trend with ramping the field from 3450
to 50 G with 4 G/s, where temperature levels are off because of the balance between heating due to the eddy
current and cooling by 3He evaporation. This suggeststhat the temperature rise during the field ramping is
a20 mK at the base temperature.

Figure 2. Schematic diagram of the 3He cryostat with bluelines showing 3He flow paths, where PTC, OVC, sorb,
and HSW, respectively, denote the pulse tube cryocooler, the outer vacuum chamber, the 3He sorption pump, and the heat switch.

Figure 3. Cooling down trend of the 3He cryostat. The originof the horizontal axis represents the time when PTC
was turned on. The plateau at 90 K is that artificiallyattained by heater control. The inset shows a magnified view near the base temperature.

139

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MLF Annual Report 2018(a)

Figure 4. Temperature trend at the base temperature observed at different ramping rates for the external
magnetic field.

3. Performance for the PSR experiment
The 3He cryostat was then loaded to the ARTEMIS
spectrometer in the S1 area to examine the performance for the PSR experiment. A slab of holmium
metal (20u20u0.3 mm) was mounted on a silver holder
made with the common design for DR at the D1 area
(Fig. 5) [1–4]. The observed P-e event rate was 95 M/
hour with 20 mmI collimator, double-pulse, and proton beam power of 300 kW. Figure 6(a) shows someexamples of PSR spectra observed at around 150 K
with a variable inner diameter for the beam collimator.
The fast-relaxing component corresponds to the signal coming from the Ho sample, while the time-independent component is backgrounds primarily from thesample holder. Curve-fit of the asymmetry [A(t)] using
a form, A(t) As exp(λt) Ab yields the signal to noise(S/N) ratio As/(As Ab) as shown in Fig. 6(b).

Figure 5. Sample holder for the 3He cryostat.

(b)

Figure 6. (a) Some examples of the μSR spectra obtained for
Ho sample (20×20×0.3 mm) using the 3He cryostat.
(b) The signal to noise ratio obtained from (a) bycurve-fit (see text).

Besides the installation of the 3He cryostat, we
worked on the maintenance of other cryostats including
their thermometers that may deviate from their original
specifications after being subjected to prolonged heat
cycles. The resistivity of some Cernox resistors (Lake
Shore Cryortronics, Inc.) was measured to update thecalibration tables. We also plan to ensure the traceability
and to keep track of the health condition of thermometers by calibration during their regular cycles.
References[1] W. Higemoto et. al., KEK Progress Report 2011-3
KEK-MSL REPORT 2010 (2011) 13.
[2] W. Higemoto et. al., KEK Progress Report 2013-3
KEK-MSL REPORT 2012 (2013) 34.
[3] W. Higemoto et. al., KEK Progress Report 2015-4
KEK-MSL REPORT 2014 (2015) 24.
[4] W. Higemoto et. al., KEK Progress Report 2018-2
KEK-MSL REPORT 2017 (2018) 9.

J. G. Nakamura1,2, A. Koda1,2, S. Nishimura1,2, H. Li2, S. Doiuchi2, A. Hashimoto2, H. Okabe2, H. Hiraishi2, and R. Kadono1,2
Muon Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK

1140

MLF Annual Report 2018

Muon Science

H-Line Construction – Recent Progress
A new beam line named H-line [1] is being constructed in the east section of Experimental Hall #1 of
the MLF. The H-line is planned to be used for various
experiments, which need high statistics, i.e. high-intensity beam and long beamtime. These characteristics
enable precise measurements such as muon g-2/EDM
experiment [2] and high-precision measurement of thehyperfine splitting of the ground state of muonium(MuSEUM experiment [3]), and is also best suited forthe rare decay search like DeeMe experiment [4], which
searches for charged lepton flavor violation (cLFV) using muonic atoms. A transmission muon microscope,
which is an unprecedented tool to obtain 3D images ofa living cell non-destructively, is planned as well.
In order to deliver a high-intensity beam to experimental areas, the H-line has a large-aperture capturesolenoid (HS1). It is located 600 mm from the muon production target and its acceptance is 108 mSr. Coils of
HS1 are wound with radiation resistant mineral insulation cables (MIC) [5]. Because MIC is a normal conducting wire, HS1 needs high electric power (a 1 MW). Other
beamline components, such as the bending magnets(HB1, HB2), the transportation solenoids (HS2, HS3), andthe focusing quadrupole triplet (HQ1–3), also have large
aperture for efficient muon transportation. Figure 1 is alayout drawing of the H-line in the first phase.

The front-end apparatuses of the H-line (HS1, HB1,
HGV1) were installed during the summer shutdowns in2012 and 2014. In 2016, all radiation shields until thefirst branch of the H-line, H1 area, were placed. A beam
blocker (HBB1) was also installed. With the beam blocker inserted, the dose rate inside the H1 area is expected
to be about 10 PSv/h, even when the beam is on.
The construction of a new electric power sub-station for the H-line has been in progress since FY2017.
The capacity of the electric sub-station is about 5 MW,
which is necessary to operate the H-line. The construction site is located in the northeast side of the MLF, as
shown in Fig. 2.
During the summer shutdown in 2017, a throughhole for electric transmission lines was drilled on the
MLF wall. The size of the aperture is 2 m u 1 m (Fig. 3).
The hole is now covered with an iron plate to keep theexperimental hall airtight. Then we started building theplatform of the electric sub-station and it was almost
completed in FY2018. Figure 4 is a picture of the electric sub-station taken in the end of FY2018. In FY2019,
electrical construction, including installation of transformers and cabling work inside the MLF building, isscheduled and all the construction of the new electric
sub-station will be completed.

Figure 2. Construction site of a new electric power sub-station. It is located outside the MLF building.

Figure 1. A layout plan of Experimental Hall #1 in the firstphase of the H-line construction.

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MLF Annual Report 2018

Figure 4. The platform of the new electric sub-station wasalmost completed in FY2018.

Figure 3. Aperture for the electric transmission lines. It is located above the carry-in entrance of the east #1
experimental hall of the MLF.

References[1] N. Kawamura, et al., Prog. Theor. Exp. Phys. 2018,
113G01 (2018).
[2] T. Mibe, et al., Chin. Phys. C 34, 745 (2010).
[3] K. Shimomura, AIP conf. proc. 1382, 245 (2011).

[4] H. Natori, et al., Nucl. Phys. B (Proc. Suppl.) 248–250,
52 (2014).
[5] H. Fujimori, et al., Nucl. Instrum. Methods Phys. Res.
Sect. A 600, 114 (2009).

T. Yamazaki1,2 and N. Kawamura1,2
Institute of Materials Structure Science, KEK; 2Muon Science Section, Materials and Life Science Division, J-PARC Center

1

142

MLF Safety

MLF Safety

MLF Annual Report 2018

Research Safety

Distribution of survey-meters to each neutron beamline
From the introduction of the low-surface contamination area, to check dose rates around the sample, andsurface contamination at sample environment devices,survey-meters are distributed at each neutron beamlines, resulting that the radiation exposure of users canbe reduced. All survey-meters are inspected and calibrated annually.
Radiological license upgrade
The applications for radiological license upgrades
in FY2018 were approved on August 22, 2018, andFebruary 4, 2019.
The following items were updated after the application approval in FY2018:(1) Addition of a sealed radioactive isotope (237Np,
10 MBq) for nuclear data measurements(2) Consideration of movable shields of a muon
beam line by re-evaluation of shielding andaddition of safety devices(3) Reduction of the storage area of radio-active
materials to install a large detector to find144

sterile neutrinos at the 3rd floor of the maintenance area in the MLF
2. Chemical safety
An annual task of the chemical-safety team is tocheck the chemical safety of user-brought chemicalmaterials, such as specimen and reagents, to evaluate
their toxicity and the stability of their actual physicalstate – powder, solid, liquid or gas. The task was performed successfully, followed by the approval of the actual materials for use by the individual beamline staffs.
As a result, the experiments were performed without
serious chemical problems. Figure 1 shows a trend forthe amount of chemical materials subjected to safety
check for over 10 years. As the beam power increases,
the number of user-brought chemical materials is also
increasing. Since a stable operation at 500 kW wasachieved for the first time during the planned beamoperation schedule for the last year, a record amountof chemical materials was brought. Over 8,000 chemical materials were brought in the MLF, which was about
10 times more than at the start of the MLF operation.
However, the total number tends to flatten recently.
Therefore, by using the last year’s data, we evaluatedthe expected number of the user-brought chemicalmaterials at 1 MW, which is full power, and we can also
estimate the total number of necessary equipment forchemical handling for sample preparation, consumables, radioactive wastes after experiments at 1 MW
operation, which is planned within several years.

䣐䣷䣯䣤䣧䣴䢢䣱䣨䢢䣥䣪䣧䣯䣫䣥䣣䣮䢢䣯䣣䣶䣧䣴䣫䣣䣮䣵

1. Radiation safety
Radiation safety for users
The low-surface contamination area has been adopted at the MLF Experimental halls from November
2016 to avoid surface-contamination problems caused
by a sample, an environmental atmosphere and so on,
and to expand the flexibility of the experiments conducted at the MLF. The number of conducted experiments using gaseous or liquid samples or atmospheres
has gradually increased.
On the other hand, samples have been radio-activated by neutron irradiations because the stable proton beam power increased to 500 kW. Especially, 60Co
(T1/2 5.271 y) and 110mAg (T1/2 249.8 d) can be foundin radio-activated samples well, resulting that the radio-active samples cannot be brought for long time. It
is required to minimize the parent nuclei 59Co and 109Ag
and/or the irradiated neutrons.
The four monitors for take-out articles worksmoothly to bring an article out from the controlledarea without significant trouble. However, hand-footclothe monitors had several troubles due to damage ofthe light shielding sheets. The devices are hoped to be
used carefully and softly.

䢺䢲䢲䢲
䢸䢲䢲䢲
䢶䢲䢲䢲
䢴䢲䢲䢲
䢲

䢴䢲䢲䢻䢴䢲䢳䢲䢴䢲䢳䢳䢴䢲䢳䢴䢴䢲䢳䢵䢴䢲䢳䢶䢴䢲䢳䢷䢴䢲䢳䢸䢴䢲䢳䢹䢴䢲䢳䢺䣛䣧䣣䣴

Figure 1. Trend of amount of user-brought chemical materials for chemical safety check from the start of the
MLF operation to the last year.

MLF Annual Report 2018

Table 1. Statistics of the common sample environment.

equipment

times

total days

7 T magnet

16

86

2 K cryostat

3

5

3He cryostat

16

95

dilution cryostat

7

41

cryostat for residual stressmeasurement2

7

GM cryo-furnace

2

10

Nb furnace

3

11

SANS furnace

1

1

Total

50

256

4. Crane safety
Throughout the year, we use cranes to change
sample environment equipment for experiments andto perform various kinds of maintenance of the neutron instruments. There are 50 t and 7.5 t cranes inexperimental hall No.1 and there are 50 t, 7.5 t and
15 t cranes in experimental hall No.2 and its extension
building. Those cranes can be operated only by crane
operators who have been licensed by the government,
additionally, they must be trained by our crane safety
staff and pass our skill test. In addition, before each individual crane operation, the crane working group must
submit a dedicated usage sheet for crane operation
whose content includes information of the suspendedload, weight, total number and method of slinging
by the crane staff. The usage sheet must be approved
before proceeding. As a result, last year, there were no
problems with the crane operations. Figure 2 shows lastyear’s statistics of use of cranes. From April to June andfrom November to March, which is the beamtime period, the MLF staffs operated cranes for changing sample
environment equipment and the frequency was almost
same. On the other hand, from June to October, which isthe period of maintenance of the neutron instruments,
the MLF staffs and constructors used cranes, therefore, cranes were used most frequently in that period.
During that time, the MLF managed the coordination of
the crane-use schedule to accommodate the needs ofstaffs and constructors.

䢴䢷䣐䣷䣯䣤䣧䣴䢢䣱䣨䢢䣥䣴䣣䣰䣧䢢䣷䣵䣣䣩䣧

3. Sample environment safety
Table 1 shows last year’s statistics of the common
sample environment, such as a magnetic field apparatus, various kinds of cryostats and various kinds of furnaces. The common sample environment equipment
was used 50 times and 256 days in total. The common
sample environment is maintained by the sample environment team whose members include JAEA, KEK and
CROSS staffs. Each common sample environment musttake a safety check by technology development section, MLF until regular operation and pass it. The safety
check examines the maximum controllable value, forexample, temperature of the equipment, the interlock
system, electrical integrity and structural integrity. If thespecifications of each common sample environment
are changed, it is necessary to conduct the safety checkagain. As a result of those measures, all common sample environment equipment operated well, and there
were no safety problems.

MLF Safety䢢䣫䣰䢯䣪䣱䣷䣵䣧䢢䣵䣶䣣䣨䣨䢢䣥䣱䣰䣵䣶䣴䣷䣥䣶䣱䣴

䢴䢲
䢳䢷
䢳䢲
䢷
䢲

䢶

䢷

䢸

䢹

䢺

䢻 䢳䢲 䢳䢳 䢳䢴 䢳
䣏䣱䣰䣶䣪

䢴

䢵

Figure 2. Trend of the total crane usage in one year.

M. Harada1, M. Ooi1, M. Sekijima1, K. Kawakami2, K. Aizawa2, A. Hori2, H. Tanaka2, W. Kambara2, M. Sawabe2, K. Suzuya3, N.
Kawamura4, Y. Sakaguchi5, R. Takahashi2, Y. Yamaguchi5, and K. Soyama6
1
Neutron Source Section, Materials and Life Science Division, J-PARC Center; 2Technology Development Section, Materials and Life Science
Division, J-PARC Center; 3Neutron Science Section, Materials and Life Science Division, J-PARC Center; 4Muon Science Section, Materials
and Life Science Division, J-PARC Center; 5Neutron Science and Technology Center, CROSS; 6Materials and Life Science Division

145

MLF Operations in 2018

MLF Operations in 2018

MLF Annual Report 2018

Beam Operation Status at MLF
Overall:
In Japanese Fiscal Year (JFY) 2018, the beam operation at the MLF started on April 1, 2018, with a beam
power of 150 kW and ended on April 2, 2019. Table 1
shows the scheduled time and availability in JFY2018.
In the schedule, 2018A switched to 2018 on November
8. Since the neutron Target #8, which was replaced in
the summer of 2018, had the helium bubbler to mitigate cavitation erosion at the target vessel, the beam
power was increased beyond 300 kW. The records ofthe beam power and the availability are shown in Fig. 1.
In JFY2018, the beam operation started with the powerof 400 kW from April 3 and was maintained at that level
until the end of April. After confirmation of the operational status with a beam power of 500 kW, the power
was increased from 400 kW to 500 kW with a doublebunch beam in time structure.
The operation continued until June 28, just before
the summer outage period. Meanwhile, continuous
beam operation with high stability and R&D for a highintensity beam operation were carried out. In order tominimize the influence on the user caused by the target
failure, we made a demonstration of the high-intensity
beam operation after user beam delivery. A beam operational demonstration with 1-MW power was successfully completed within 1 hour on July 3. The memorialphoto is shown in Fig. 2. After the summer outage period, the beam operation resumed on October 20. Due tothe failure of the helium bubbler, the beam power was
decreased from 500 kW to 300 kW. After the bubbler

Figure 2. Memorial photo after the completed demonstration of 1-MW beam operation on June 3, 2018.

Table 1. Run cycle, scheduled time, and availability.

Run

Duration

Scheduled time (h)Beamtime (h)Availability (%)

79
80
81
2018A
2018B
OverallApr 3 – Jun 29
Oct 22– Dec 16
Jan 22 – Mar 25
Apr 3 – Nov 7
Nov 8 – Mar 25

1812
1188
1294
2163
2131
4294

1669.01120.11191.51974.92287.64179.4

92.1
94.3
92.1
92.0
93.4
92.7

Figure 1. Beam power trend (blue line) at the MLF and availability per day (red line).

148

MLF Annual Report 2018

MLF Operations in 2018

Table 2. Events that stopped the beam and made the daily availability of less than 80%.

Stop dateCause of beam stop

4/12
4/13
4/22
5/14
5/15
5/27
6/20
6/21
10/23
10/28
12/7
1/25 and 1/26
2/21 and 2/22
3/10
3/12
3/14

RCS charge exchange foil failure
RCS RF failure
LINAC water flow shortage
LINAC vaccum pump failure
LINAC water flow shortage
3NBT magnet layer short failure
LINAC water leak at klystron gallery
Oarai facility radiation failure event
RCS kicker magnet #2 power supply failure
RCS kicker magnet #5 power supply failure
RCS kicker magnet #3 power supply failure
RCS shift bump magnet power supply failure
LINAC ion source failure and replacement
RCS RF power supply failure
LINAC water flow shortage and the power supply for the klystron
3-50BT bending magnet (B15D) failure surveirance

was repaired, the operation was continued with thebeam power of 500 kW.
Since no significant failures occurred in JFY2018,the achieved average availability was as high as 92.7%.
In the past, a relatively long beam shutdown period was
required to complete the purification of the cryogenic
system for the neutron moderator. In the summer of
2016, the impurities in the loop of the cryogenic systemwere removed completely; after that, the periodical
purification is not required. Thus, a long uninterrupted
work period of 4,179 h was attained in JFY2018.
The beam operation was stopped on several occasions due to minor failures. Typical causes of the beamstops with daily availability of less than 80% are summarized in Table 2 and described below.
LINAC:
During JFY2018, a shortage of water flow for themagnet and power supplies at LINAC occurred threetimes, on April 22, May 15, and March 12, respectively. A
vacuum pump at LINAC for the beam dump (90-degree
beam dump) failed on May 14. A controller of the highvoltage power supply to the klystron also failed. Afterthe replacement of the controller, the beam operation
was resumed. The ion source at LINAC was stopped
on February 21. It took a long time to replace the ion
source, which caused the most prolonged downtime ofthe operation in JFY2018.

Stop durationfor each event [h]
3.3
8.1
4.5
8.7
10.2
13.3
18.9
3.3
5.6
8.4
6.8
13.4
21.3
8.0
12.4
15.4

3-GeV Rapid Cycling Synchrotron (RCS):The power supplies to the kicker magnet at RCS
failed three times, on October 23 and 28, and December
7, respectively. Also, the power supply for the shift
bump magnet failed on January 25. Power supplies for
the RCS RF also failed on April 13 and March 10.
Beam transport from RCS to MLF (3NBT) :A malfunction of the quadruple magnet’s coil happened on May 27 at 3NBT. Without the use of the failed
magnet, the beam transport was resumed after thechange of the beam optics at 3NBT.
30-GeV Synchrotron (MR):A beam-bending magnet failed at the 3–50 BT,
which delivers the beam from the RCS to MR. The coilalso had malfunction due to the layer short. Without theusage of the bending magnet, the beam cannot continue the delivery. In order to survey the magnet failure
preciously, the beam operation to MLF was stopped.
Other facilities:
The outside facility of J-PARC, Oarai, had a failure
event involving radiation safety on June 21. JAEA decided to stop the operation of all facilities before thesafety of each facility was confirmed. After the confirmation of the safety, the beam operation was resumed
on June 22.
149

MLF Operations in 2018

MLF Annual Report 2018

Users at the MLF
In fiscal year (FY) 2018, the MLF was running stably with beam power of 500 kW throughout the year,
except for the first two weeks’ 400-kW operation from
April 3 and the first two weeks’ 300-kW operation from
October 22. That led to an average availability up to
92.7%. In addition, the 1-MW beam test was successfully operated for one hour on July 3, 2018, before thesummer maintenance period. The total number of users of the neutron and muon experimental facilities in
FY2018 reached 965, which was the highest number todate.
The trend for the number of users at the MLF since
the start of the operations in FY2008 is summarized inTable 1 and Fig. 1.

Table 1. The number of domestic and foreign users by fiscal year.
FY2008Domestic
Users
NeutronMuon

FY2009Foreign
Users

Domestic
Users

12

303

0

38

Foreign
Users

Domestic
Users

107

18

Muon

432

2

42

Foreign
Users

Domestic
Users

113

476

59

Foreign
Users

Domestic
Users

44

238

8

21

Foreign
Users

Domestic
Users

83

108

742

16

149

Muon (Japanese)

Muon (Foreigners)

13

18
12
95
FY2008
FY
Y200
20
008
08

38
14
303

432

628

FY20
20
0 09
FY2009FY20010
FY2010FY202011
FY2011

FY20012
FY2012

Domestic
Users

50
50

80

399

10

50

Foreign
Users

449
50
61
11

Foreign
Users

965
789

176
161

30

146

30

108

185

15

15
146

900

176

750
600

59
83

450

711
744
476

742

789

300
150

FY2013
FY2013FFY20
14FY2014FY2015FY2015FYY2016
FY2016FY201
17FY2017

Figure 1. The number of domestic and foreign users by fiscal year.

150

DomesticUsers

FY2018

83
10

399

238

Foreign
Users

Foreign
Users

56

16

78
113
11

2
21
21

46

149

46
80

42
44

2

FY2013708

185

Neutron (Foreigners)

10

2

628

179

Neutron (Japanese)

8

21

927

99
10

DomesticUsers

FY2017852
744

Foreign
Users

23

FY201683

FY2012

259

50

69
13

FY2011

476

559

91
78

14

FY2015824
711

Domestic
Users

40

18
FY2014

NeutronForeign
Users

317

95

DomesticUsers

FY20100
FYY2018
FY2018

MLF Annual Report 2018

MLF Operations in 2018

MLF Proposals Summary – FY2018
Table 1. Breakdown of Proposals Numbers for the 2018 Rounds.
2018A
Beamline

Instrument

BL01 4D-Space Access Neutron Spectrometer - 4SEASONS
BL02 Biomolecular Dynamics Spectrometer - DNA
BL03 Ibaraki Biological Crystal Diffractometer - iBIX
BL04

2018B

Full Year

Submitted

Approved

Submitted

Approved

Submitted

Approved

GU

GU

GU

GU

PU/S

IU

PU/S

IU

18(0)

10(0)

18(0)

13(0)

1

1

1

1
1

14(1)

12(1)

25(2)

13(2)

2

1

2

(100E)‡

4

2

2

1

0

0

0

0

(E)†

0

0

0

0

33

0

33

0

6

4

10

4

1

1

1

1

3

3

5

5

0

0

0

0

Accurate Neutron-Nucleus Reaction Measurement Instrument ANNRI

BL05 Neutron Optics and Physics - NOP
BL06 Neutron Resonance Spin Echo Spectrometers - VIN ROSE

2

2

7

4

0

0

0

0

BL08 Super High Resolution Powder Diffractometer - S-HRPD

8

7

9

8(0)

0

0

0

0

BL09 Special Environment Neutron Power Diffractometer - SPICA

4

1

2

2

0

0

0

0

BL10 Neutron Beamline for Observation and Research Use - NOBORU

4

4

10

7

2

1

2

1

BL11 High-Pressure Neutron Diffractometer - PLANET

9(0)

7(0)

7(0)

7

0

1

0

1

BL12 High Resolution Chopper Spectrometer - HRC

8

6

7

7

1

0

1

0

BL14 Cold-neutron Disk-chopper Spectrometer - AMATERAS

34

17

24

13

3

1

3

1

BL15 Small and Wide Angle Neutron Scattering Instrument - TAIKAN

34(3)

17(3)

36(3)

22(3)

3

3

3

3

20

18

20

19

0

1

0

1

16(0)

11(0)

20(1)

14(1)

2

3

2

3

24(0)

12(0)

18(0)

5(0)

1

2

1

2

20

18

22

15(0)

1

1

1

1

BL16

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

BL17 Polarized Neutron Reflectometer - SHARAKU
BL18

Extreme Environment Single Crystal Neutron Diffractometer SENJUBL19 Engineering Diffractometer - TAKUMI(100E)

‡

8

7

7

7

0

0

0

0

31

31

31

31

25

0

25

0

BL21 High Intensity Total Diffractometer - NOVA

15

13

25

19

0

0

0

0

BL22 Energy Resolved Neutron Imaging System - RADEN

13(1)

12(1)

20(2)

15(2)

0

3

0

3

BL23 Polarization Analysis Neutron Spectrometer - POLANO

0

0

0

0

0

0

0

0

BL20 Ibaraki Materials Design Diffractometer - iMATERIA

(E)†

D1

Muon Spectrometer for Materials and Life Science Experiments D1

9(1)

6(1)

15(1)

4(1)

0

1

0

1

D2

Muon Spectrometer for Basic Science Experiments - D2

8(0)

6(0)

9(0)

6(0)

0

1

0

1

S1

General purpose PSR spectrometer - ARTEMIS

13(0)

12(0)

25(2)

18(2)

0

1

0

1

UA

Muon U

0

0

0

0

0

1

0

1

325

238

374

266

75

23

75

23

Total

GU : General Use
PU : Project Use or Ibaraki Pref. Project Use
IU : Instrument Group Use† : Ibaraki Pref. Exclusive Use Beamtime (β 80% in FY2018)‡ : J-PARC Center General Use Beamtime (100β 20% in FY2018)( ) : Proposal Numbers under New User Promotion or P-type proposals (D1,D2) in GU

Table 2. Proposals Numbers of Long Term Proposal.
Application FY

Submitted

Approved

2017

24

8

2018

9

5

S : S-type Proposals

In addition, you can check the MLF experimental Report 2018 via thefollowing links:
http://j-parc.jp/researcher/MatLife/en/lists/2018A.html
http://j-parc.jp/researcher/MatLife/en/lists/2018B.html
http://j-parc.jp/researcher/MatLife/en/lists/2018AB.html
http://j-parc.jp/researcher/MatLife/en/lists/2018LTP.html

151

MLF Operations in 2018

MLF Annual Report 2018

900
800

199

700
142
Proposals

231

293

600

278

395

500

Not Approved

400

126

42
300

45

20
200

309

34
67

214

FY2008FY2009

100

460

422

469

255

Approved

321

353

FY2015FY2016507

607

FY2017FY20180
FY2010FY2011FY2012FY2013

FY2014

Proposal Round

Figure 1. MLF Proposal Numbers over Time.

JAEA
84
10%

KEK
37
5%

CROSS
32
4%

Universies (Japan)
Universies (Japan)
344
43%

Foreign Organizaons
150
19%Companies (Japan)
Research Instutes (Japan)
Foreign Organizaons
JAEA
KEK
CROSS

Research Instutes (Jaapan)
37
Companies (Japan)
4%
122
15%

Figure 2. Origin of Submitted Proposals by affiliation - FY2018.

P9
P7 13
43 2%
7%

P6
49
8%
P5
80
13%

Q1
41
6%

P1 :Materials Science and Engineering
P2 :Energy Science and High-Pressure ScienceP3 :Soft Matter, Biomaterials and Liquids
P4 :Magnetism and Strongly Correlated Electron Systems

Q2
35
5%
P1
130
21%

(Elastic Scattering)P5 :Magnetism and Strongly Correlated Electron Systems(Inelastic Scattering)

P4
62
10%

P3
119
19%

P2
56
9%

P6 :Fundamental and Nuclear Physics, Instrumentation, Imaging
P7 :Industrial Applications
P8 :(Reserved)
P9 :Trial Use Access Program
Q1 :Electronic Properties of Matter & Hydrogen in Matter
Q2 :Hydrogen in Matter & General Applications

Figure 3. Submitted Proposals by Sub-committee/Expert Panel - FY2018.

152

MLF Annual Report 2018

MLF Operations in 2018

MLF Division Staff 2018
Toshiji Kanaya (Head)

Kazuya Aizawa (Deputy Head)

Kazuhiko Soyama (Deputy Head)

Eiichi Wakai

Toshiya Otomo (Deputy Head)

Izumi Kuwahara

Yasuhiro Miyake (Deputy Head)

Neutron Source Section*: additional duties<JAEA>
Katsuhiro Haga (Leader)

Hideyuki Nemoto

Noriyuki Morikawa

Kenji Sakai (Sub-Leader)

Akihiko Watanabe

Shizuka Yoshinari

Masahide Harada

Hideki Muto

Miyuki Hoshino

Makoto Teshigawara

Kouhei Hanano

Hiroshi Takada *Hiroyuki Kogawa

Mitsuaki Sekijima

Shoichi Hasegawa *Tomokazu Aso

Katsuhiro Aoyagi

Eiichi Wakai *Motoki Ooi

Yoshinori Kikuchi

Shin-ichiro Meigo *Takashi Naoe

Masakazu Nakamura

Hidetaka Kinoshita *Takashi Wakui

Hidemitsu Hosokawa

Kenichi Oikawa *Masakazu Seki

Atsushi Akutsu

Tetsuya Kai *Shiho Masuda

Toshiyuki Yasuhra

Hiroyuki Uehara *Motonori Takagi

Hiromi Inoue

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

Hiroyuki Aoki

Hiroshi Nakagawa *Yukinobu Kawakita (Sub-Leader)

Takuro Kawasaki

Hideo Harada *Kentaro Suzuya

Kousuke Hiroi

Atsushi Kimura *Ryoichi Kajimoto

Maiko Kofu

Shoji Nakamura *Takanori Hattori

Naoki Murai

Yosuke Toh *Mitsutaka Nakamura

Yoshichika Seki

Mariko Segawa *Stefanus Harjo

Takayuki Yamashita

Masahide Harada *Kenichi Oikawa

Tatsuya Kikuchi

Kazuya Aizawa *Takashi Ohhara

Takeshi Harada

Masao Watanabe *Takenao Shinohara

Hideaki Isozaki

Dai Yamazaki *Tetsuya Kai

Kazuhiro Aoyama

Hiroshi Suzuki *Seiko Kawamura

Misono Fujii

Satoshi Morooka *Shinichi Takata

Naoko Shimizu

Atsushi Moriai *Ryoji Kiyanagi

Mariko Ohtake

Kazuo Kurihara *Kaoru Shibata

Miho Igarashi

Tarou Tamada *Asami Sano

Itaru Tamura *Yuu Hirano *Yasuhiro Inamura

Kouji Kaneko *153

MLF Operations in 2018

MLF Annual Report 2018

<KEK>
Shinichi Ito (Sub-Leader)

Norifumi Yamada

Kazutaka Ikeda

Hideki Seto

Takashi Honda

Masao Yonemura

Toshiya Otomo *Naokatsu Kaneko

Masato Hagihala

Takashi Kamiyama

Shuki Torii

Fumiya Nemoto

Hitoshi Endo

Hidetoshi Oshita

Hiraku Saito

Testuya Yokoo

Kaoru Taketani

Seiji Sugai

Takashi Ino

Kenji Mishima

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

Kazuhiro kawakami

Tatsuya Nakamura *Takayuki Oku (Sub-Leader)

Hiromichi Tanaka

Yasuhiro Inamura *Takeshi Nakatani

Masaki Sawabe

Masahide Harada *Masao Watanabe

Yukiko Nagai

Tomokazu Aso *Yuhua Su

Kenji Sakai *Seiko Kawamura *Takuya Okudaira

Tetsuya Kai *Fumiaki Kono *The Dang Vu

Hiroyuki Kogawa *Rumi Shimizu *Wataru Kambara

Motoki Ooi *Tatsuhito Matsuo *Akihiro Hori

Kentaro Suzuya *Satoru Fujiwara *Hideaki Takahashi

Mitsutaka Nakamura *Motoyasu Adachi *Ryuta Takahashi

Shinichi Takata *Shigeki Arai *Wu Gong

Kaoru Sakasai *Yoshiteru Yonetani *Setsuo Sato

Takashi Ino *Hiroshi Fujimori *Tomohiro Seya

Naokatsu Kaneko *Shunsuke Makimura *Testuya Yokoo *Kaoru Taketani *Shuki Torii *Naritoshi Kawamura *<KEK>

Neutron Instrumentation Section*: additional duties<JAEA>

154

Kaoru Sakasai (Leader)

Tatsuya Nakamura

Yukiko Uno

Dai Yamazaki

Ryuji Maruyama *Masumi Ebine *Kentaro Toh

Noriaki TsutsuiMLF Annual Report 2018

Muon Science Section

MLF Operations in 2018*: additional duties<KEK>
Ryosuke Kadono (Leader)

Shiro Matoba

Masatoshi Hiraishi

Naritoshi Kawamura (Sub-Leader)

Soshi Takeshita

Hirotaka Okabe

Yasuhiro Miyake *Hiroshi Fujimori

Motonobu Tanpo

Koichiro Shimomura

Shunsuke Makimura

Tatsuhiko Tachibana

Patrick Strasser

Yasuo Kobayashi

Hua Li

Akihiro Koda

Yutaka Ikedo

Masato Tabe

Takayuki Yamazaki

Junpei Nakamura

Shogo Doiuchi

Yu OishiTaihei Adachi

Akiko Hashimoto

Yukinori Nagatani

Shoichiro Nisimura

Izumi Umegaki<JAEA>
Wataru Higemoto *Takashi Ito *155

MLF Operations in 2018

MLF Annual Report 2018

CROSS Staff 2018
Director

Hideaki Yokomizo

Science Coordinators
Kazuhisa Kakurai

Makoto Hayashi

Mikio Kataoka

Takashi Noma

Research & Development Division*: additional duties

Jun-ichi Suzuki (Head)<BL15 Group><Technical Support Group>

Kenichi Funakoshi (Deputy Head)

Kazuki Ohishi (Leader)

Koji Kiriyama (Leader)

Tsukasa Miyazaki *(Deputy Head)

Jun-ichi Suzuki *Takayoshi Ito (Sub-Leader)

Sayaka Suzuki

Hiroki Iwase

Yoshifumi Sakaguchi

Yukihiko Kawamura

Hiroshi Kira
Motoyuki Ishikado<BL01 Group>
Kazuya Kamazawa (Leader)<BL17 Group>

Nobuo Okazaki

Kazuhiko Ikeuchi

Noboru Miyata (Leader)

Shuoyuan Zhang

Kazuki Iida

Kazuhiro Akutsu

Makoto Kobayashi

Takayasu Hanashima

Satoshi Kasai
Toshiaki Morikawa<BL02 Group>
Masato Matsuura (Leader)<BL18 Group>

Hideyuki Hiramatsu

Takeshi Yamada

Akiko Nakao (Leader)

Yutaka Ebara

Taiki Tominaga

Koji Munakata

Kentaro Moriyama

Yoshihisa Ishikawa

Hiroshi Arima
Yasuji Masuda<BL11 Group>
Kenichi Funakoshi *(Leader)<BL22 Group>

Keiichi Ohuchi

Jun AbeHirotoshi Hayashida (Leader)

Masae Sahara

Shinichi Machida

Joseph Don Parker
Yoshihiro Matsumoto

Safety Division156*: additional duties

Yasuhiro Yamaguchi (Head)

Tazuko Mizusawa *Koji Kiriyama *Masae Sahara *MLF Annual Report 2018

Utilization Promotion Division

MLF Operations in 2018*: additional duties

Junichi Sato (Head)

Miho Igarashi

Junko Ohta

Tsukasa Miyazaki (Deputy Head)Toshiki Asai (Leader)

Yutaka Ebara *Atsuko Irie

Emi Goto

Takayoshi Ito *Seiya Konishi (Leader)

Taeko Ishikawa

Nobuo Okazaki *Tazuko Mizusawa

Maya Endo

Administration Division
Michihiko Murasawa (Head)

Rei Ohuchi

Mutsumi Shiraishi

Takashi Hikita (Leader)

Tomoko Sakuma

Shinobu Matsumoto157

MLF Operations in 2018

MLF Annual Report 2018

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)
Director General
KEK

President
JAEA

Director
J-PARC

J-PARC
CenterPresident
CROSS

Director
CROSS

CollaboraonCommiee

Neutron research Center(JAEA/KEK)

RegisteredInstuon(CROSS)All except Public Beamlines Public Beamlines Only

MLF Advisory
Board

Muon Instrument
Proposal Rev. Comm.

Muon Science
Proposal Rev. Comm.

Selecon
Commiee

Task Forces

All except Contract
Beamlines

Contract Beamlines
Only

All except Public
Beamlines

Public Beamlines Only

Neutron Instrument
Proposal Rev. Comm.

Contract Beamline
Evaluaon Comm.

Neutron Science
Proposal Rev. Comm.

Proposal
Evaluaon Comm.

Joint Meeng

Muon
Instrument
Proposals

Joint Meeng

Neutron Instrument
Proposals
Muon Program
Advisory Comm.

Muon Scienﬁc Proposals

Public Beamlines Only
All except Public Beamlines
JAEA Research
CROSS Development
Neutron Program
Proposal Advisory Proposal Evaluaon
Advisory
Commiee
PanelCommiee
Joint Meeng

Neutron Scienﬁc Proposals
UniﬁedAccess Point

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

158

MLF Annual Report 2018

MLF Operations in 2018Materials and Life Science Facility Advisory Board

Kenji Nakajima

Japan Atomic Energy Agency

Kazuya Aizawa

Japan Atomic Energy Agency

Toshiya Otomo

High Energy Accelerator Research
Organization

Hiroshi Amitsuka

Hokkaido University
Yoshiharu Sakurai

Taka-hisa Arima

The University of TokyoJapan Synchrotron Radiation
Research Institute

Masatoshi Futakawa

Japan Atomic Energy Agency

Taku Sato

Tohoku University

Ryosuke KadonoHigh Energy Accelerator Research
Organization

Hideki Seto

High Energy Accelerator Research
Organization

Kazuhisa Kakurai

Comprehensive Research
Organization for Science and Society

Mitsuhiro Shibayama The University of Tokyo

Takashi Kamiyama

High Energy Accelerator Research
Organization

Kazuhiko Soyama

Japan Atomic Energy Agency

Masaaki Sugiyama(chair)

Kyoto University

Jun-ichi Suzuki

Comprehensive Research
Organization for Science andSociety

Takashi Kamiyama

Hokkaido University

Toshiji Kanaya

High Energy Accelerator Research
Organization

Yukinobu Kawakita

Japan Atomic Energy Agency

Atsushi Takahara

Kyushu University

Takamitsu Kohzuma

Ibaraki University

Masayasu Takeda

Japan Atomic Energy Agency

Yoji Koike

Tohoku University

Toshio Yamaguchi

Fukuoka University

Kenya Kubo

International Christian University

Term: through March 31, 2021

Yasuhiro Miyake

High Energy Accelerator Research
Organization

Neutron Science Proposal Review Committee
Hiroyuki Kagi

The University of Tokyo

Ryosuke KadonoHigh Energy Accelerator Research
Organization

Toshiji Kanaya

High Energy Accelerator Research
Organization

Yoshiaki Kiyanagi

Nagoya University

Tsukasa Miyazaki

Comprehensive Research
Organization for Science and Society

Kenji Nakajima

Japan Atomic Energy Agency

Kenji Ohoyama

Ibaraki University

Hideki Seto

High Energy Accelerator Research
Organization

Shinichi Shamoto

Japan Atomic Energy Agency

Yuichi Shimakawa

Kyoto University

Hirohiko Shimizu

Nagoya University

Masaaki Sugiyama(chair)

Kyoto University

Masayasu Takeda

Japan Atomic Energy Agency

Ichiro Tanaka

Ibaraki University

Term: through September 30, 2019

Muon Science Proposal Review Committee

Katsuyuki Fukutani

The University of Tokyo

Tadashi Adachi

Sophia University

Wataru Higemoto

Japan Atomic Energy Agency

Kenta Amemiya

High Energy Accelerator Research
Organization

Adrian Hillier

Rutherford Appleton Laboratory

Ryosuke Kadono

Hiroshi Amitsuka

Hokkaido University

High Energy Accelerator Research
Organization

Hidehito Asaoka

Japan Atomic Energy Agency

Toshiji Kanaya

High Energy Accelerator Research
Organization

Toshiyuki Azuma

Institute of Physical and Chemical
Research

Naritoshi Kawamura

High Energy Accelerator Research
Organization

159

MLF Operations in 2018

MLF Annual Report 2018

Yasushi Kino

Tohoku University

Toshiya Otomo

Akihiro Koda

High Energy Accelerator Research
Organaization

High Energy Accelerator Research
Organization

Hideki Seto

High Energy Accelerator Research
Organization

Tatsushi Shima

Osaka University

Koichiro Shimomura

High Energy Accelerator Research
Organaization

Jun Sugiyama

Toyota Central R&D Labs.

Masaaki Sugiyama

Kyoto University Research Reactor
Institute

Kenya Kubo (chair)International Christian University

Roderick Macrae

Marian University

Yasuyuki Matsuda

University of Tokyo

Tsutomu Mibe

High Energy Accelerator Research
Organization

Yasuhiro Miyake

High Energy Accelerator Research
Organization

Kenji Nakajima

Japan Atomic Energy Agency

Chihiro OhmoriHigh Energy Accelerator Research
Organization

Hideki Tou

Kobe University

Term: through March 31, 2019

Proposal Evaluation Committee

Shinichi Shamoto

Japan Atomic Energy Agency

Hiroyuki Kagi

The University of Tokyo

Yuichi Shimakawa

Kyoto University

Toshiji Kanaya

High Energy Accelerator Research
Organization

Hirohiko Shimizu

Nagoya University

Nagoya University

Masaaki Sugiyama(chair)

Kyoto University

Yoshiaki Kiyanagi
Tsukasa Miyazaki

Comprehensive Research
Organization for Science and Society

Ichiro Tanaka

Ibaraki University

Kenji Ohoyama

Ibaraki University

Selection Committee

160

Toshiyuki Takayanagi Saitama University

Term: through September 30, 2019

Yoshiharu Sakurai

Japan Synchrotron Radiation
Research InstituteTaku Sato

Tohoku University

Taka-hisa Arima

The University of Tokyo

Yasuhiro Iye (chair)Japan Society for Promotion of
Science

Mitsuhiro Shibayama The University of Tokyo

Takashi Kamiyama

Hokkaido University

Masaaki Sugiyama

Kyoto University

Hiroyuki Kishimoto

Sumitomo Rubber Industries, LTD.

Atsushi Takahara

Kyushu University

Hideaki Kitazawa

Research Center for Strategic
Materials

Shinji Tsuneyuki

The University of Tokyo

Toshio Yamaguchi

Fukuoka University

Yoji Koike

Tohoku University

Takamitsu Kohzuma

Ibaraki University

Term: through March 31, 2021

MLF Annual Report 2018

MLF Operations in 2018

Neutron Advisory Committee (NAC)
NAC convened 18–19 February, 2019 at the J-PARC Research Center, TokaiGroup photo of NAC

Neutron Advisory Committee (18–19 Feb. 2019)

Robert McGreevy (chair)

Rutherford Appleton Laboratory

Bertrand Blau

Paul Scherrer Institut (PSI)

Mark Wendel

Oak Ridge National Laboratory

oshiaki Kiyanagi

Nagoya University

Christiane Alba Simionesco

The Laboratoire Leon Brilloin

Jamie Schulz

Australian Nuclear Science and Technology Organization

Andreas Schreyer

European Spallation Source

Sung-Min Choi

Korea Advanced Institute of Science and Technology

Yoshie Otake

Institute of Physical and Chemical Research

Masaaki Sugiyama

Kyoto University

Christian Rüegg

Paul Scherrer Institut

Muon Advisory Committee (MAC)
MAC convened 1 - 2 March, 2019 at the KEK Tokai Campus, TokaiGroup photo of MAC
Prokscha Thomas (chair)

Muon Advisory Committee (1–2 Mar. 2019)
The Paul Scherrer InstituteMartin Månsson

KTH Royal Institute of Technology

Andrew Macfarlane

The University of British Columbia

Klaus Kirch

ETH Zurich and Paul Scherrer InstituteKenya Kubo

International Christian University

Tadayuki Takahashi

The University of Tokyo

Takashi Nakano

Osaka University

Hiroshi Amitsuka

Hokkaido University

161

MLF Operations in 2018

MLF Annual Report 2018

Workshops, Conferences, Seminars and Schools in 2018
Conferences held jointly by J-PARC MLF andCROSS
The 21th Conference on Superionic Conductor(The 70th Solid State Ionics Society of Japan)
1–2 Jun. 2018, IBARAKI Quantum Beam ResearchCenter, Ibaraki

User Group Meeting on TOF near Backscattering
Spectrometer DNA 201812 Oct. 2018, IBARAKI Quantum Beam Research Center,
Ibaraki

The 1st Workshop on Deuterium Materials
10, Jul. 2018, Nagoya Institute of Technology, Aichi
2018 Meeting on J-PARC MLF Industrial Use
23–24 Jul. 2018, Akihabara Convention Hall, Tokyo

Photo of User Group Meeting on TOF near Backscattering
Spectrometer DNA 20182018 Z-Code Intermediate Level Training Course
16 Nov. 2018, Essam Kanda Hall, Tokyo

Photo of the 2018 Meeting on J-PARC MLF Industrial Use(photo courtesy of J-PARC Center)

J-PARC Workshop: Deuterated Materials
Enhancing Neutron Science for Structure Function
Applications
15–16 Jan. 2019, IBARAKI Quantum Beam ResearchCenter, Ibaraki

The 6th Workshop on Pulsed Neutron Imaging
10 Oct. 2018, Essam Kanda Hall, Tokyo
User Group Meeting on MLF Spectrometers
DIRECTION 2018
10–11 Oct. 2018, IBARAKI Quantum Beam ResearchCenter, Ibaraki

Photo of the J-PARC Workshop(photo courtesy of J-PARC Center)

Group photo of User Group Meeting on MLF Spectrometers
DIRECTION 20182018 Z-Code Beginner Level Training Course
2 Feb. 2019, Essam Kanda Hall, Tokyo
Meeting on Evaluation Technology of Reinforced
Concrete Using Neutron
15 Feb. 2019, Tokyu Construction Co., Ltd., Tokyo

162

MLF Annual Report 2018

3rd Workshop on the Collaborative Use of Large
Research Institutions and the KEI Super Computer
2018
25 Feb. 2019, Public Relation Center SPring-8, Hyogo
2018 Quantum Beam Science Festival (The 10th MLF
Symposium and The 36th PF Symposium)
12–13 Mar. 2019, Tsukuba International Congress
Center, Ibaraki

MLF Operations in 2018

Workshops and Seminars held by CROSS andother organizations
The 21th CROSSroads Workshop“Dynamics and Neutron Scattering of Biological
Materials and Hydrated Water”
2 Jul. 2018, IBARAKI Quantum Beam Research Center
and KEK Tokai Campus, Ibaraki

Group photo of the 2018 Quantum Beam Science Festival(photo courtesy of J-PARC Center)

Group photo of the CROSSroad 21 (photo courtesy of CROSS)

2018 1st Workshop on Structural Biology
2 Sep. 2018, Essam Kanda Hall, Tokyo

Workshops held by KEK
Workshop for Negative Muon Research
1–3 Jul. 2018 KEK Tokai Campus, Ibaraki
Workshop for Neutron Spin Echo Research (BL06)
30 Oct. 2018, KEK Tokai Campus, Ibaraki
Structural Study for Functional Materials using
SPICA (BL09)
26 Nov. 2018, KEK Tsukuba Campus, Ibaraki
Fundamental Physics with Pulsed Cold Neutrons(BL05)
21 Dec. 2018, Nagoya University, Nagoya
High-Resolution Neutron Powder Diffraction
Method using SuperHRPD (BL08)25 Dec. 2018, KEK Tsukuba Campus, Ibaraki

2018 1st Workshop on Polymer Science under
Humidity Control
1 Oct. 2018, TKY Conference Center, Tokyo
2018 1st Workshop on Residual Stress and Strain
9 Oct. 2018, Essam Kanda Hall, Tokyo
2018 2nd Workshop on iMATERIA “Neutron
Scattering of Electrode Material on Charge/
discharge”
18 Oct. 2018, Essam Kanda Hall, Tokyo
Neutron Experiment Technique Training Course
2 Nov. 2018, Essam Kanda Hall, Tokyo
Workshop on Magnetc Materials
9 Nov. 2018, Essam Kanda Hall, Tokyo
Workshop on Non-destructive Visualization andAnalysis Methods
14 Nov. 2018, Essam Kanda Hall, Tokyo

163

MLF Operations in 2018

MLF Annual Report 2018

Meeting on Deuterium Labeled Compound for
Neutron Science
15 Nov. 2018, J-PARC Center and IBARAKI Quantum
Beam Research Center, Ibaraki

Schools in 2018
Hello Science from J-PARC: Investigation“Water” Deep in the Earth with Neutrons
14 May. 2018, iVil, Tokai
The 3rd Neutron and Muon School
20–24 Nov. 2018, J-PARC Center and IBARAKI Quantum
Beam Research Center, Ibaraki

Group photo of the CROSSroad 21(photo courtesy of J-PARC Center)2018 Workshop on Materials Science
14 Dec. 2018, Essam Kanda Hall, Tokyo

Group photo of the 3rd Neutron and Muon School(photo courtesy of J-PARC Center)2018 Workshop on Soft Matter Neutron Scattering
25 Dec. 2018, Essam Kanda Hall, Tokyo
2018 Workshop on Battery Materials
15 Jan. 2019, KENKYUSHA EIGO Center, Tokyo
2018 Workshop on Surfaces and Interfaces
30 Jan. 2019, Essam Kanda Hall, Tokyo
2018 Workshop on Metallographic Structure
22 Feb. 2019, Essam Kanda Hall, Tokyo
2018 Workshop on Liquids and Amorphous
Materials
11 Mar. 2019, Tsukuba International Congress Center,
Ibaraki
5th Symposium on the Collaborative Use of Large
Research Institutions and the KEI Super Computer
2018
15 Mar. 2018, Akihabara UDX, Tokyo
2018 2nd Workshop on Residual Stress and Strain
19 Mar. 2019, Essam Kanda Hall, Tokyo
2018 2nd Workshop on Structural Biology
27 Mar. 2019, Essam Kanda Hall, Tokyo

164

Hello Science from J-PARC: Observing the Force
Supporting Reinforced Concrete by Neutrons
30 Nov. 2018, iVil, Tokai
Hello Science from J-PARC: Visualization of Lithium
Ion Secondary Battery using Neutron Beam
22 Feb. 2019, iVil, TokaiMLF Annual Report 2018

MLF Operations in 2018

Award List
51st The Atomic Energy Society of Japan Award : Best
Paper Award
Measurements of neutron total and capture cross sectionsof 241Am with ANNRI at J-PARC
K. Terada, A. Kimura, T. Nakao (2019-03-21)
The Journal of Nuclear Science and Technology Most
Cited Article Award 2018
Neutron-capture cross-sections of 244Cm and 246Cm
measured with an array of large germanium detectors in
the ANNRI at J-PARC/MLF
K. Terada, A. Kimura, T. Nakao, S. Nakamura, K. Mizuyama,
N. Iwamoto, O. Iwamoto, H. Harada, T. Katabuchi,
M. Igashira, T. Sano, Y. Takahashi, C.H. Pyeon, S. Fukutani,
T. Fujii, T. Yagi, K. Takamiya & J. Hori (2019-03-21)
JSNS President’s Choice
Clarification of refrigerant boiling behavior in an evaporator
utilizing neutron imaging.
T. Fuse, T. Okamura, S. Inoue, T. Matsuno, R. Iwata,
T. Yamauchi, T. Shimazu, Y. Matsumoto, T. Shinohara,
T. Kai (2018-12-05)
The18th JSNS Poster Prize
Expansion of application of neutron atomic resolution
holography
S. Uechi (2018-12-04)
The18th JSNS Poster Prize
Simulation Software for Neutron Holography Apply to B
doped 6H-SiC
Y. Fukumoto (2018-12-04)
73rd Ceramic Society of Japan Awards foradvancements in ceramic science and technology(2018)
High-performance ferroelectric perovskites by controlling
defect and polarization structures
Y. Kitanaka (2018-11-29)
73rd The Ceramic Society of Japan Academic Award(2018)
Materials design and new function development of polar
perovskites
Y. Noguchi (2018-11-29)

JAEA President Award 2018 [ R & D Achievement
Prize]
Construction and Leading Research of the Energy-Resolved
Neutron Imaging System, RADEN
T. Shinohara, T. Kai, K. Oikawa, M. Segawa, T. Nakatani,
M. Harada, M. Ooi, K. Hiroi, Y.H. Su, Y. Kiyanagi,
T. Kamiyama, H. Sato, J.D. Parker, H. Hayashida,
Y. Matsumoto (2018-10-01)
School of High Energy Accelerator Science Dean’sAward
The investigation of negative thermal expansion andmagnetic structure in La0.5Ba0.5CoO3x by neutron powder
diffraction.
Z.J. Tan ( 2018-09-29)
APS Fellow
K. Tanaka (2018-09)
Jacek Grochowski Memorial Poster Prize
Local structure observation of Sm doped RB6 (R: rareearth) by white neutron atomic resolution holography
S. Uechi (2018-08-27)
The Adhesion Society of Japan Award
Study on molecular picture of adhesive interface
K. Tanaka (2018-06)
Award of The Society of Fiber Science and Technology,
Japan
A Novel Design Concept of Bio-scaffolds Based on
Dimension Controlled Polymers
H. Matsuno (2018-06)
Atom Indonesia Best Paper Award 2017(I-AIBPA
2017)
Synthesis, Structural and Magnetic Properties of
La0.5Ba0.5CoO2.75+x
Z.J. Tan, P. Miao, Y. Ishikawa, M. Hagihala, S. Lee, S. Torii,
M. Yonemura, T. Kamiyama
Atom Indonesia 44 49 (2018) (2017-12-5)

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MLF Operations in 2018

MLF Annual Report 2018

MLF Publication 2018
1

S. Lee, M.-C. Lee, Y. Ishikawa, P. Miao, S. Torii, C. Won, K. Lee, N. Hur,
D.-Y. Cho, and T. Kamiyama
Crystal and Magnetic Structures of La2CoPtO6 Double Perovskite
ACS Omega 3 11624 (2018)13

2

N. Yano, T. Yamada, T. Hosoya, T. Ohhara, I. Tanaka, N. Niimura, andK. Kusaka
Status of the neutron time-of-flight single-crystal diffraction dataprocessing software STARGazer
Acta Crystallographica Section D STRUCTURAL BIOLOGY D74
1041–1052 (2018)

T. Takami, Y. Morita, M. Yonemura, Y. Ishikawa, S. Tanaka, M. Mori, T.
Fukunaga, and E. Matsubara
Appearance of Lithium-Ion Conduction in a La–Li–Co–O Band
Insulator: Possible Route to Oxide Electrolyte
Applied Energy Materials 1 2546 (2018)

14

J.W. Bae, J.B. Seol, J. Moon, S.S. Sohn, M.J. Jang, H.Y. Um, B.-J. Lee,and H.S. Kim
Exceptional phase-transformation strengthening of ferrous mediumentropy alloys at cryogenic temperatures
Acta Materialia 161 388–399 (2018)

C.H. Lee, A. Nishida, T. Hasegawa, H. Nishiate, H. Kunioka, S. OhiraKawamura, M. Nakamura, K. Nakajima, and Y. Mizuguchi
Effect of rattling motion without cage structure on lattice thermal
conductivity in LaOBiS2−xSex
Applied Physics Letters 112 023903 (2018)

15

Z.J. Tan, P. Miao, Y. Ishikawa, M. Hagihala, S. Lee, S. Torii, M.
Yonemura, and T. Kamiyama
Synthesis, Structural and Magnetic Properties of La0.5Ba0.5CoO2.75+x
Atom Indonesia 44 49 (2018)16

M. Hirai, S. Ajito, M. Sugiyama, H. Iwase, S. Takata, N. Shimizu, N.
Igarashi, A. Martel, and L. Porcar
Direct evidence for the effect of glycerol on protein hydration andthermal structural transition
Biophys. J. 115 313–327 (2018)17

Y. Kameda, Y. Amo, T. Usuki, Y. Umebayashi, K. Ikeda, and T. Otomo
Neutron Diffraction Study on Partial Pair Correlation Functions of
Water at Ambient Temperature
Bull. Chem. Soc. Jpn. 91 1586–1595 (2018)18

H. Nishihara, H. Fujimoto, H. Itoi, K. Nomura, H. Tanaka, M.T.
Miyahara, P.A. Bonnaud, R. Miura, A. Suzuki, N. Miyamoto, N.
Hatakeyama, A. Miyamoto, K. Ikeda, T. Otomo, and T. Kyotania
Graphene-based ordered framework with a diverse range of carbon
polygons formed in zeolite nanochannels
Carbon 129 854–862 (2018)19

K. Kataoka and J. AkimotoHigh ionic conductor member of garnet‐type oxide Li6.5La3Zr1.5Ta0.5O12
Chem. Electro. Chem. 5 2551–2557 (2018)20

M. Yoshimoto, Y. Yoshida, Y. Noda, S. Koizumi, S. Takata, J. Suzuki, A.
Hoshikawa, T. Ishigaki, S. Ozeki, and T. Iiyama
Mesoscopic investigation of an “immiscible” cyclohexane and water
micro-mixture in carbon micropores by contrast variation small-angle
neutron scattering
Chem. Lett. 47 336–339 (2018)

21

A. Chanyshev, K. Litasov, S. Rashchenko, A. Sano-Furukawa, H. Kagi,
T. Hattori, A. Shatskiy, A. Dymshits, I. Sharygin, and Y. Higo
High-Pressure - High-Temperature Study of Benzene: Refined Crystal
Structure and New Phase Diagram up to 8 GPa and 923K
Crystal Growth & Design 18 3016–3026 (2018)22

Y. Muraba, S. Iimura, S. Matsuishi, H. Hiramatsu, T. Honda, K. Ikeda,
T. Otomo, and H. Hosono
Phase transition in CaFeAsH: bridging 1111 and 122 iron-based
superconductors
Dalton Trans. 47 12964–12971 (2018)23

N. Naganawa, T. Ariga, S. Awano, M. Hino, K. Hirota, H. Kawahara,
M. Kitaguchi, K. Mishima, H.M. Shimizu, S. Tada, S. Tasaki, and A.
UmemotoA Cold/Ultracold Neutron Detector using Fine-grained Nuclear

3

4

5

6

7

8

9

10

11

12

166

K. Tomiyasu, N. Ito, R. Okazaki, Y. Takahashi, M. Onodera, K. Iwasa, T.
Nojima, T. Aoyama, K. Ohgushi, Y. Ishikawa, T. Kamiyama, S. OhiraKawamura, M. Kofu, and S. Ishihara
Quantum paramagnet near spin-state transition
Advanced Quantum Technologies 2018 1800057 (2018)
K. Suekuni, C.-H. Lee, H.I. Tanaka, E. Nishibori, A. Nakamura, H.
Kasai, H. Mori, H. Usui, M. Ochi, T. Hasegawa, M. Nakamura, S. OhiraKawamura, T. Kikuchi, K. Kaneko, H. Nishiate, K. Hashikuni, Y. Kosaka,
K. Kuroki, and T. Takabatake
Retreat from stress: rattling in a planar coordination
Advansed Materials 30 1706230 (2018)
K. Ikeuchi, K. Nakajima, S. Ohira-Kawamura, R. Kajimoto, S.
Wakimoto, and M. Fujita
Al-impurity-induced magnetic excitations in heavily over-doped
La1.7Sr0.3Cu0.95Al0.05O4
AIP Advances 8 101318 (2018)
T. Okuda, R. Kajimoto, M. Noda, and H. Kuwahara
Schottky specific heat of the lightly Mn-substituted electron-doped
SrTiO3
AIP Advances 8 101339 (2018)
T. Yokoo, S. Itoh, N. Kaneko, M. Fujita, T. Ino, M. Ohkawara, and M.
Sakaguchi
Ready to Roll? Time to Launch POLANOAIP Conf. Proc. 1969 050001 (2018)
S. Itoh, T. Yokoo, T. Masuda, H. Yoshizawa, M. Soda, S. Ibuka, Y. Ikeda,
M. Yoshida, T. Hawai, D. Kawana, R. Sugiura, T. Asami, Y. Kawamura,T. Shinozaki, and Y. Ihata
High Resolution Chopper Spectrometer HRC and Neutron Brillouin
Scattering
AIP Conf. Proc. 1969 050002 (2018)
R. Kajimoto, K. Sato, Y. Inamura, and M. Fujita
Instrumental Resolution of the Chopper Spectrometer 4SEASONS
Evaluated by Monte Carlo Simulation
AIP Conf. Proc. 1969 050004 (2018)
Y. Fukushima, K. Yamada, K. Tamura, and K. Shibata
Dynamic of organic species in organo-clay / polypropyrene composite
by quesi-elastic neutron scattering
Appl. Clay. Sci. 155 15–19 (2018)
H. Iwase, T. Ogura, H. Sakuma, K. Tamura, and Y. Fukushima
Structural investigation of hectorite aqueous suspensions by dielectric

microscopy and small-angle neutron scattering coupling withrheological measurement
Appl. Clay. Sci. 157 24–30 (2018)

MLF Annual Report 2018

Emulsion with Spatial Resolution less than 100 nm
European Physical Journal C 78 959 (2018)
24

25

26

27

28

Y. Seki, T. Shinohara, J.D. Parker, W. Ueno, T. Samoto, W. Yashiro, A.
Momose, Y. Otake, and Y. Kiyanagi
Efficient phase imaging using wavelength-resolved neutron TalbotLau interferometry with TOF method
Europhysics Letters 123 12002 (2018)
K. Mishima, H. Sumino, T. Yamada, S. Ieki, N. Nagakura, H. Otono,
and H. Oide
Accurate determination of the absolute 3He/4He ratio of a synthesizedhelium standard gas (Helium Standard of Japan, HESJ): Towards
revision of the atmospheric 3He/4He ratio
Geochemistry, Geophysics, Geosystems 19 3995–4005 (2018)
T. Nakamura, T. Kawasaki, K. Toh, M. Ebine, A. Birumachi, and K.
SakasaiA sub-millimeter spatial resolution scintillation neutron detector fortime-of-flight neutron diffraction imaging
IEEE Nuclear science symposium and medical imaging conference,
conference record N07-197 (2018)
W. Liao, M. Hashimoto, S. Manabe, Y. Watanabe, S. Abe, K. Nakano,
H. Sato, T. Kin, K. Hamada, M. Tampo, and Y. Miyake
Measurement and Mechanism Investigation of Negative and Positive
Muon-Induced Upsets in 65nm Bulk SRAMs
IEEE Trans. Nucl. Sci. 65 1734 (2018)
S. Manabe, Y. Watanabe, W. Liao, M. Hashimoto, K. Nakano, H. Sato,T. Kin, S. Abe, K. Hamada, M. Tampo, and Y. Miyake
Negative and Positive Muon-Induced Single Event Upsets in 65-nm
UTBB SOI SRAMs
IEEE Trans. Nucl. Sci. 65 1742 (2018)

MLF Operations in 2018

Inhomogeneity of local packing density and atomic bonding of
Ni67Zr33 amorphous alloy
J. Alloys. Comp. 732 585–592 (2018)36

Y. Nagata, T. Nishikawa, M. Suginome, S. Sato, M. Sugiyama, L.
Porcar, A. Martel, R. Inoue, and N. Sato
Elucidating the solvent effect on the switch of the helicity ofpoly(quinoxaline-2,3-diyl)s: A conformational analysis by small-angle
neutron scattering
J. Am. Chem. Soc. 140 2722–2726 (2018)37

A. Shinozaki, K. Komatsu, H. Kagi, C. Fujimoto, S. Machida, A. SanoFurukawa, and T. Hattori
Behavior of intermolecular interactions in a-glycine under highpressure
J. Chem. Phys. 148 044507 (2018)

38

F. Nemoto, M. Kofu, M. Nagao, K. Ohishi, S. Takata, J. Suzuki, T.
Yamada, K. Shibata, T. Ueki, Y. Kitazawa, M. Watanabe, and O.
Yamamuro
Neutron scattering studies on short- and long-range layer structuresand related dynamics in imidazolium-based ionic liquids
J. Chem. Phys. 149 054502 (2018)

39

K. Fujii, M. Yashima, K. Hibino, M. Shiraiwa, K. Fukuda, S. Nakayama,
N. Ishizawa, T. Hanashima, and T. OhharaHigh oxide-ion conductivity by the overbonded channel oxygens in
Si-deficient La9.565(Si5.826䕕0.174)O26 apatite without interstitial oxygens
J. Mater. Chem. A 6 10835–10846 (2018)40

H. Abe, T. Yamada, and K. Shibata
Dynamic properties of nano-confined water in an ionic liquid
J. Mol. Liq. 264 54–57 (2018)

41

A. Mori, H. Mamiya, M. Ohnuma, J. Ilavsky, K. Ohishi, J. Wozniak, A.
Olszyna, N. Watanabe, J. Suzuki, H. Kitazawa, and M. Lewandowska
Manufacturing and characterization of Ni-free N-containing ODS
austenitic alloy
J. Nucl. Mater. 501 72–81 (2018)42

M. Hirai, S. Ajito, H. Iwase, S. Takata, N. Ohta, N. Igarashi, and N.
Shimizu
Restoration of myoglobin native fold from its initial state of amyloid
formation by trehalose
J. Phys. Chem. B 122 11962–11968 (2018)

29

T. Suwa, T. Hemmi, T. Saito, Y. Takahashi, K. Norikiyo, V. Luzin, H.
Suzuki, and S. Harjo
Evaluation of Thermal Strain Induced in Components of Nb3Sn Strand
During CoolingIEEE Transactions on Applied Superconductivity 28 1–4 (2018)30

Y. Higaki, Y. Inutsuka, H. Ono, N.L. Yamada, Y. Ikemoto, and A.
Takahara
Counteranion-Specific Hydration States of Cationic Polyelectrolyte
BrushesInd. Eng. Chem. Res. 57 5268–5275 (2018)
43

31

K. Asano, H. Kim, K. Sakaki, K. Jimura, S. Hayashi, Y. Nakamura, K.
Ikeda, T. Otomo, A. Machida, and T. Watanuki
Structural Variation of Self-Organized Mg Hydride Nanoclusters in
Immiscible Ti Matrix by Hydrogenation
Inorg. Chem. 57 11831–11838 (2018)

Y. Kameda, S. Maeda, Y. Amo, T. Usuki, K. Ikeda, and T. Otomo
Neutron Diffraction Study on the Structure of Hydrated Li(+) in Dilute
Aqueous Solutions
J. Phys. Chem. B 122 1695–1701 (2018)

44

F. Takeiri, T. Yamamoto, N. Hayashi, S. Hosokawa, K. Arai, J. Kikkawa,
K. Ikeda, T. Honda, T. Otomo, C. Tassel, K. Kimoto, and H. Kageyama
A Fluorine-rich Perovskite Oxyfluoride AgFeOF2
Inorg. Chem. 57 6686–6691 (2018)

S. Ajito, H. Iwase, S. Takata, and M. Hirai
Sugar-mediated stabilization of protein against chemical or thermal
denaturation
J. Phys. Chem. B 122 8685–8697 (2018)

45

W. Gong, K. Aizawa, S. Harjo, R.X. Zheng, T. Kawasaki, J. Abe, T.
Kamiyama, and N. Tsuji
Deformation behavior of as-cast and as-extruded Mg97 Zn1Y2alloys
during compression, as tracked by in situ neutron diffraction
International Journal of Plasticity 111 288–306 (2018)

J. Kijima, Y. Shibuya, K. Katayama, T. Itoh, H. Iwase, Y. Fukushima, M.
Kubo, and A. Yamaguchi
Structural characterization of myoglobin molecules adsorbed withinmesoporous silicas
J. Phys. Chem. C 122 15567–15574 (2018)

46

S. Taminato, M. Hirayama, K. Suzuki, K.S. Kim, K. Tamura, and R.
Kanno
Reversible Structural Changes and High-Rate Capability of Li3PO4Modified Li2RuO3 for Lithium-Rich Layered Rocksalt Oxide Cathodes
J. Phys. Chem. C 122 16607 (2018)47

H. Kadowaki, M. Wakita, B. Fak, J. Ollivier, S. Ohira-Kawamura, K.
Nakajima, H. Takatsu, and M. Tamai
Continuum excitation and pseudospin wave in quantum spin-liquidand quadrupole ordered states of Tb2+xTi2-xO7+y

32

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K. Yoshida, T. Inoue, M. Torigoe, T. Yamada, K. Shibata, and T.
Yamaguchi
Thermal behavior, structure, dynamic properties of aqueous glycine
solutions confined in mesoporous silica MCM-41 investigated by x-ray
diffraction and quasi-elastic neutron scattering
J . Chem. Phys. 149 124502 (2018)
K. Itoh, J. Saida, and T. Otomo

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MLF Annual Report 2018

J. Phys. Soc. Jpn. 87 064704 (2018)
48

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52

Y. Oba, T. Shinohara, H. Sato, Y. Onodera, K. Hiroi, Y.H. Su, and M.
Sugiyama
Imaging Measurement of Neutron Attenuation by Small-Angle
Neutron Scattering Using Soller Collimator
J. Phys. Soc. Jpn. 87 094004 (2018)
T. Nakajima, V. Ukleev, K. Ohishi, H. Oike, F. Kagawa, S. Seki, K.
Kakurai, Y. Tokura, and T. Arima
Uniaxial-stress effects on helimagnetic orders and skyrmion latticein Cu2OSeO3
J. Phys. Soc. Jpn. 87 094709 (2018)
K. Iwasa, F. Iga, T. Moyoshi, A. Nakao, and T. Ohhara
Magnetic-Ordering Propagation Vectors of Terbium Hexaboride
Revisited
J. Phys. Soc. Jpn. 87 64705 (2018)
D. Kawana, M. Soda, M. Yoshida, Y. Ikeda, T. Asami, R. Sugiura, H.
Yoshizawa, T. Masuda, T. Hawai, S. Ibuka, T. Yokoo, and S. Itoh
YUI and HANA: Control and Visualization Programs for HRC in J-PARC
J. Phys.: Conf. Ser. 1021 012014 (2018)

53

Y. Inamura, T. Ito, and J. Suzuki
Applications of the differential events reading method at MLF, J-PARC
J. Phys.: Conf. Ser. 1021 012015 (2018)

54

S. Itoh, T. Yokoo, T. Masuda, H. Yoshizawa, M. Soda, M. Yoshida, T.
Hawai, D. Kawana, R. Sugiura, T. Asami, and Y. Ihata
Improvement for Neutron Brillouin Scattering Experiments on High
Resolution Chopper Spectrometer HRC
J. Phys.: Conf. Ser. 1021 012028 (2018)55

R. Kajimoto, M. Nakamura, Y. Inamura, K. Kamazawa, K. Ikeuchi, K.
Iida, M. Ishikado, N. Murai, H. Kira, T. Nakatani, S. Ohira-Kawamura,
R. Takahashi, N. Kubo, W. Kambara, K. Nakajima, and K. Aizawa
Status report of the chopper spectrometer 4SEASONS
J. Phys.: Conf. Ser. 1021 012030 (2018)

56

57

58

59

60

168

N. Metoki, H. Yamauchi, H.S. Suzuki, H. Kitazawa, K. Kamazawa, K.
Ikeuchi, R. Kajimoto, M. Nakamura, and Y. Inamura
Neutron Inelastic Scattering Study of the f-Electron States in NdPd5Al2
J. Phys. Soc. Jpn. 87 084708 (2018)

Y. Miki, H. Yamaguchi, Y. Iizawa, H. Shishido, K.M. Kojima, K. Oikawa,
M. Harada, S. Miyajima, M. Hidaka, T. Oku, K. Soyama, and T. Ishida
Neutron signal features of Nb-based kinetic inductance detector with
10B convertor
J. Phys.: Conf. Ser. 1054 012054 (2018)
T. Koyama and T. Ishida
Electrodynamic theory for the operation principle of a superconducting
kinetic inductance stripline detector
J. Phys.: Conf. Ser. 1054 012055 (2018)
Y. Iizawa, H. Yamaguchi, Y. Miki, K. Nishimura, H. Shishido, K.M.
Kojima, K. Oikawa, M. Harada, S. Miyajima, M. Hidaka, T. Oku, K.
Soyama, T. Koyama, and T. Ishida
Physical characteristics of delay-line current-biased kinetic inductancedetector
J. Phys.: Conf. Ser. 1054 012056 (2018)
K. Ninomiya, M. Kitanaka, A. Shinohara, M. Tampo, Y. Miyake, Y.
Sakai, and M.K. Kubo
Muonic X-ray measurements on mixtures of CaO/MgO and Fe3O4/
MnO
J. Radioanal. Nucl. Chem. 316 1107–1111 (2018)
N.V. Mdlovu, Y. Chen, K.-S. Lin, M.-W. Hsu, S.S.-S. Wang, C.-M. Wu,
Y.-S. Lin, and K. Ohishi
Multifunctional nanocarrier as a potential micro-RNA delivery vehicle

for neuroblastoma treatment
J. Taiwan Inst. Chem. Eng. 96 526–537 (2018)
61

Y. Kitanaka, M. Ogino, Y. Noguchi, M. Miyayama, A. Hoshikawa,and T. Ishigaki
Crystal Structure and ferroelectric polarization of tetragonal(Bi1/2Na1/2)TiO3–12BaTiO3Japanese Journal of Applied Physics 57 11UD05 (2018)

62

T. Okuchi, N. Tomioka, P. Narangoo, and K. Shibata
Quasielastic neutron scattering of brucite to analyse hydrogentransport on the atomic scale
Journal of Applied Crystallography 51 1564–1570 (2018)63

T. Kawasaki, Y. Inamura, T. Ito, T. Nakatani, S. Harjo, W. Gong, andK. Aizawa
Stroboscopic time-of-flight neutron diffraction during cyclic testing
using the event data recording system at J-PARC
Journal of Applied Crystallography 51 630–634 (2018)

64

P.G. Xu, S. Harjo, M. Ojima, H. Suzuki, T. Ito, W. Gong, S.C. Vogel, J.
Inoue, Y. Tomota, K. Aizawa, and K. Akita
High stereographic resolution texture and residual stress evaluation
using time‐of‐flight neutron diffraction
Journal of applied crystallography 51 746–760 (2018)

65

K. Mochiki, T. Uragaki, J. Koide, Y. Kushima, J. Kawarabayashi, A.
Taketani, Y. Otake, Y. Matsumoto, Y.H. Su, K. Hiroi, T. Shinohara, and
T. Kai
Pulsed-neutron imaging by a high-speed camera and center-ofgravity processing
Journal of Instrumentation 13 C01038 (2018)

66

S. Takada, T. Okudaira, F. Goto, K. Hirota, A. Kimura, M. Kitaguchi, J.
Koga, T. Nakao, K. Sakai, H.M. Shimizu, T. Yamamoto, and T. Yoshioka
Characterization of germanium detectors for the measurementof the angular distribution of prompt γ-rays at the ANNRI in the
MLF of the J-PARC
Journal of Instrumentation 13 P02018 (2018)67

Y. Iwasaki, N. Matsui, K. Suzuki, Y. Hinuma, M. Yonemura, G.
Kobayashi, M. Hirayama, I. Tanaka, and R. Kanno
Synthesis, crystal structure, and ionic conductivity of hydride ionconducting Ln2LiHO3 (Ln = La, Pr, Nd) oxyhydrides
Journal of Materials Chemistry A 6 23457–23463 (2018)

68

T. Wakui, E. Wakai, T. Naoe, Y. Shintaku, T. Li, K. Murakami, K.
Kanomata, H. Kogawa, K. Haga, H. Takada, and M. Futakawa
Recent studies for structural integrity evaluation and defect inspectionof J-PARC spallation neutron source target vessel
Journal of Neuclear Materials 506 3–11 (2018)

69

H. Muta, R. Nishikane, Y. Ando, J. Matsunaga, K. Sakamoto, S. Harjo,
T. Kawasaki, Y. Ohishi, K. Kurosaki, and S. Yamanaka
Effect of hydrogenation conditions on the microstructure andmechanical properties of zirconium hydride
Journal of Nuclear Materials 500 145–152 (2018)

70

K. Terada, A. Kimura, T. Nakao, S. Nakamura, K. Mizuyama, N.
Iwamoto, O. Iwamoto, H. Harada, T. Katabuchi, M. Igashira, T. Sano,
Y. Takahashi, C.H. Pyeon, S. Fukutani, T. Fujii, T. Yagi, K. Takamiya,and J. Hori
Measurements of neutron total and capture cross sections of 241Am
with ANNRI at J-PARC
Journal of Nuclear Science and Technology 55 1198–1211 (2018)71

T. Tsuchiya, R. Kobayashi, T. Kubota, K. Saito, K. Ono, T. Ohhara, A.
Nakao, and K. Takanashi
Mn2VAl Heusler alloy thin films: Appearance of antiferromagnetismand exchange bias in a layered structure with Fe
Journal of Physics D: Applied Physics 51 065001 (2018)

MLF Annual Report 2018

72

H. Matsuda, S. Meigo, and H. Iwamoto
Measurement of activation cross sections of the target and the proton
beam window materials at J-PARC
Journal of Physics: Conference Series 1021 012016 (2018)

73

K. Nakajima, S. Ohira-Kawamura, T. Kikuchi, M. Kofu, Y. Kawakita, Y.
Inamura, W. Kambara, K. Aoyama, D. Wakai, M. Harada, and M. Ooi
Recent issues encountered by AMATERAS: A cold-neutron disk-chopper
spectrometer
Journal of Physics: Conference Series 1021 012031 (2018)74

T. Kai, T. Uchida, H. Kinoshita, M. Seki, M. Ooi, T. Wakui, K. Haga, Y.
Kasugai, and H. Takada
Off-gas processing system operations for mercury target vessel
replacement at J-PARC
Journal of Physics: Conference Series 1021 012042 (2018)75

M. Teshigawara, M. Harada, M. Ooi, and H. Takada
Present fabrication status of spare moderators and reflector in J-PARC
spallation neutron source
Journal of Physics: Conference Series 1021 012061 (2018)76

T. Aso, M. Teshigawara, S. Hasegawa, H. Muto, K. Aoyagi, K. Nomura,and H. Takada
Recovery of helium refrigerator performance for cryogenic hydrogensystem at J-PARC MLF
Journal of Physics: Conference Series 1021 012085 (2018)

77

78

79

80

81

82

83

84

K. Ikeuchi, T. Kikuchi, K. Nakajima, R. Kajimoto, S. Wakimoto, andM. Fujita
Fe-impurity-induced magnetic excitations in heavily over-doped
La1.7Sr0.3Cu0.95Fe0.05O4
Journal of Physics: Conference Series 969 012024 (2018)
Y. Idemoto, T. Hiranuma, N. Ishida, and N. Kitamura
Effect of operating temperature on local structure during firstdischarge of 0.4Li2MnO3-0.6LiMn1/3Ni1/3Co1/3O2 electrodes
Journal of Power Sources 378 198–208 (2018)
T. Ohkubo
Insights from ab initio molecular dynamics simulations for a
multicomponent oxide glass
Journal of the American Ceramic Society 101 1122–1134 (2018)
N. Matsui, G. Kobayashi, K. Suzuki, A. Watanabe, A. Kubota, Y.
Iwasaki, M. Yonemura, M. Hirayama, and R. Kanno
Ambient pressure synthesis of La2LiHO3 as a solid electrolyte for ahydrogen electrochemical cell
Journal of the American Ceramic Society 102 3228–3235 (2018)
H. Yamashita, T. Broux, Y. Kobayashi, F. Takeiri, T. Zhu, M.A. Hayward,
K. Fujii, M. Yashima, T. Murakami, and H. Kageyama
Chemical Pressure-induced Anion Order-disorder Transition in LnHO
Enabled by Hydride Size Flexibility
Journal of the American Chemical Society 140 11170–11173 (2018)
W. Uno, K. Fujii, E. Niwa, S. Torii, P. Miao, T. Kamiyama, and M.
Yashima
Experimental visualization of oxide-ion diffusion paths in pyrochloretype Yb2Ti2O7
Journal of the Ceramic Society of Japan 126 341–345 (2018)
K. Fujii and M. Yashima
Discovery and development of BaNdInO4 - A brief review Journal of the Ceramic Society of Japan 126 852–859 (2018)
T. Matsushita, T. Muro, F. Matsui, N. Happo, S. Hosokawa, K.
Ohoyama, A. Sato-Tomita, Y.C. Sasaki, and K. Hayashi
Principle and Reconstruction Algorithm for Atomic-Resolution
Holography
Journal of the Physical Society of Japan 87 061002 (2018)

MLF Operations in 2018

85

K. Oyama, M. Sugishima, K. Tanabe, A. Mitsuda, H. Wada, K.
Ohoyama, T. Matsukawa, Y. Yoshida, A. Hoshikawa, T. Ishigaki, andK. Iwasa
Neutron Diffraction Studies on Valence Ordering Compound YbPd
Journal of the Physical Society of Japan 87 114705 (2018)86

S. Ohira-Kawamura, K. Tomiyasu, A. Koda, D.P. Sari, R. Asih, S. Yoon,
I. Watanabe, and K. Nakajima
Magnetic Properties of One-Dimensional Quantum Spin System
Rb2Cu2Mo3O12 Studied by Muon Spin Relaxation
JPS Conf. Proc. 21 011007 (2018)87

M. Fujita, K.M. Suzuki, S. Asano, A. Koda, H. Okabe, and R. KadonoμSR Study of Magnetism in the As-Prepared and Non-Superconducting
T*-La0.9Eu0.9Sr0.2CuO4
JPS Conf. Proc. 21 011026 (2018)88

T. Sumura, T. Ishimoto, H. Kuwahara, K. Kurashima, Y. Koike, I.
Watanabe, M. Miyazaki, A. Koda, R. Kadono, and T. Adachi
Reduction Effects on the Cu-Spin Correlation in the Electron-Doped
T'-Cuprate Pr1.3-xLa0.7CexCuO4+δ (x = 0.10)
JPS Conf. Proc. 21 011027 (2018)

89

K. Nishimura, K. Matsuda, N. Nunomura, T. Namiki, S. Lee, D.
Hatakeyama, W. Higemoto, Y. Miyake, T. Matsuzaki, G. Itoh, K. Ihara,
H. Toda, and M. Yamaguchi
Muon Spin Relaxation of an Al–3.4%Zn–1.9%Mg alloy
JPS Conf. Proc. 21 011030 (2018)90

M. Mihara, H. Araki, M. Mizuno, K. Shimomura, W. Higemoto, K.
Sugita, K. Atsushi, M. Kondo, Y. Tanaka, T. Matsuzaki, R. Kadono, W.
Sato, T. Nakano, and T. Fukuda
μSR Study on Hydrogen Behavior in Palladium
JPS Conf. Proc. 21 011031 (2018)

91

T. Kiyotani, M. Kobayashi, I. Tanaka, and N. Niimura
Visualization of proton and electron transfer processes of abiochemical reaction by μSR
JPS Conf. Proc. 21 011037 (2018)

92

A.D. Pant, Y. Sugawara, H. Nakanishi, E. Torikai, W. Higemoto, K.
Shimomura, and K. Nagamine
Theoretical Calculations of Charge States and Stopping Sites of Muons
in Glycine and Triglycine
JPS Conf. Proc. 21 011038 (2018)

93

G.D. Liu, Y.G. Chen, A.H. Morrison, A. Koda, P.W. Percival, and K.
GhandiSupercritical Water Experimental Setup for μSR
JPS Conf. Proc. 21 011039 (2018)94

I. Umegaki, Y. Higuchi, H. Nozaki, K. Ninomiya, M.K. Kubo, M. Tampo,
K. Hamada, S. Doiuchi, P. Strasser, N. Kawamura, Y. Miyake, and J.
Sugiyama
Detection of Li in Li-ion Battery Electrode Materials by Muonic X-ray
JPS Conf. Proc. 21 011041 (2018)

95

K. Ninomiya, M.K. Kubo, P. Strasser, A. Shinohara, M. Tampo, N.
Kawamura, and Y. Miyake
Isotope Identification of Lead by Muon Induced X-ray and Gamma-ray
Measurements
JPS Conf. Proc. 21 011043 (2018)96

G. Yabu, M. Katsuragawa, M. Tampo, K. Hamada, A. Harayama, Y.
Miyake, S. Oshita, S. Saito, G. Sato, T. Takahashi, S. Takeda, and S.
Watanabe
Imaging of Muonic X-ray of Light Elements with a CdTe Double-Sided
Strip Detector
JPS Conf. Proc. 21 011044 (2018)

97

P. Strasser, K. Shimomura, and H.A. Torii
Possibility of New Precise Measurements of Muonic Helium Atom HFS

169

MLF Operations in 2018

MLF Annual Report 2018

at J-PARC MUSEJPS Conf. Proc. 21 011045 (2018)
98

G. Yoshida, K. Ninomiya, M. Inagaki, M. Toyoda, J. Aoki, N. Kawamura,Y. Miyake, and A. Shinohara
Development of Muonic Atom Beam Extraction System and First
Evaluation by Intense Negative Muon Beam of J-PARC MUSEJPS Conf. Proc. 21 011046 (2018)

109 S. Tada, S. Awano, M. Hino, K. Hirota, H. Kawahara, M. Kitaguchi, K.
Mishima, N. Naganawa, H.M. Shimizu, S. Tasaki, and A. Umemoto
Development of High Spatial Resolution Cold/Ultra-Cold Neutron
Detector Using Nano Imaging Tracker
JPS Conf. Proc. 22 011023 (2018)99

Y. Miyake, K. Shimomura, N. Kawamura, A. Koda, P. Strasser, K.M.
Kojima, H. Fujimori, S. Makimura, Y. Ikedo, Y. Kobayashi, J. Nakamura,Y. Oishi, S. Takeshita, T. Adachi, A.D. Pant, H. Okabe, S. Matoba, M.
Tampo, M. Hiraishi, K. Hamada, S. Doiuchi, W. Higemoto, T.U. Ito,and R. Kadono
J-PARC Muon Facility, MUSEJPS Conf. Proc. 21 011054 (2018)

110 T. Uragaki, J. Koide, J. Kawarabayashi, K. Mochiki, Y. Matsumoto, Y.H.
Su, K. Hiroi, T. Shinohara, and T. Kai
Evaluation of high-frame-rate camera with digital accumulation
system combined with neutron color image intensifier for energy
resolved neutron imaging
JPS Conf. Proc. 22 011027 (2018)

100 D. Tomono, M. Fukuda, K. Hatanaka, W. Higemoto, Y. Kawashima,
K.M. Kojima, Y. Kuno, Y. Matsuda, T. Matsuzaki, Y. Miyake, K.
Miyamoto, Y. Morita, T. Motoishi, Y. Nakazawa, K. Ninomiya, R.
Nishikawa, S. Ohta, A. Sato, K. Shimomura, K. Takahisa, Y. Weichao,and M.L. Wong
Muon Beamline Commissioning and Feasibility Study for μSR at a New
DC Muon Beamline, MuSIC-RCNP, Osaka University
JPS Conf. Proc. 21 011057 (2018)
101 S. Makimura, S. Matoba, N. Kawamura, Y. Matsuzawa, M. Tabe, H.
Aoyagi, H. Kondo, Y. Kobayashi, H. Fujimori, Y. Ikedo, R. Kadono, A.
Koda, K.M. Kojima, Y. Miyake, J.G. Nakamura, Y. Oishi, H. Okabe, K.
Shimomura, and P. Strasser
Perspective of Muon Production Target at J-PARC MLF MUSEJPS Conf. Proc. 21 011058 (2018)
102 S. Matoba, S. Makimura, N. Kawamura, Y. Matsuzawa, M. Tabe, Y.
Kobayashi, R. Kadono, and Y. Miyake
Renovation of a Scraper Unit of a Muon Production Target at J-PARC
JPS Conf. Proc. 21 011059 (2018)
103 A.D. Pant, T. Adachi, Y. Ikedo, Y. Oishi, J. Nakamura, P. Strasser, K.M.
Kojima, S. Makimura, N. Kawamura, A. Koda, T.U. Ito, W. Higemoto,K. Shimomura, R. Kadono, Y. Miyake, and E. Torikai
Transportation of Ultra Slow Muon on U-line, MLF, J-PARC
JPS Conf. Proc. 21 011060 (2018)

170

RADEN
JPS Conf. Proc. 22 011022 (2018)

111 M. Segawa, K. Oikawa, T. Kai, T. Shinohara, H. Hayashida, Y.
Matsumoto, J.D. Parker, T. Nakatani, K. Hiroi, Y.H. Su, and Y. Kiyanagi
Spatial Resolution Test Targets Made of Gadolinium and Gold forConventional and Resonance Neutron Imaging
JPS Conf. Proc. 22 011028 (2018)
112 K. Hiroi, T. Shinohara, H. Hayashida, J.D. Parker, K. Oikawa, Y.H. Su,
T. Kai, and Y. Kiyanagi
Development of a Polarization Analysis Method for Visualization of
the Magnetic Field Distribution in a Small Electric Transformer using
Pulsed Polarized Neutron Imaging
JPS Conf. Proc. 22 011030 (2018)
113 K. Mishima, S. Awano, Y. Fuwa, F. Goto, C.C. Haddock, M. Hino, M.
Hirose, K. Hirota, S. Ieki, S. Imajo, T. Ino, Y. Iwashita, R. Katayama,
H. Kawahara, M. Kitaguchi, R. Kitahara, J. Koga, A. Morishita, T.
Nagae, N. Nagakura, N. Naganawa, N. Oi, H. Oide, H. Otono, Y. Seki,
D. Sekiba, T. Shima, H.M. Shimizu, W.M. Snow, N. Sumi, H. Sumino,
S. Tada, K. Taketani, S. Tasaki, T. Tomita, A. Umemoto, T. Yamada, S.
Yamashita, M. Yokohashi, and T. Yoshioka
Fundamental physics activities with pulsed neutron at J-PARC(BL05)
JPS Conf. Proc. 22 011033 (2018)
114 N. Sumi, H. Otono, T. Yoshioka, K. Mishima, and Y. Makida
Precise Neutron Lifetime Measurement with a Solenoidal CoilJPS Conf. Proc. 22 011036 (2018)

104 P. Strasser, A. Koda, K.M. Kojima, T.U. Ito, H. Fujimori, Y. Irie, M. Aoki, Y.
Nakatsugawa, W. Higemoto, M. Hiraishi, H. Li, H. Okabe, S. Takeshita,
K. Shimomura, N. Kawamura, R. Kadono, and Y. Miyake
Status of the New Surface Muon Beamline at J-PARC MUSEJPS Conf. Proc. 21 011061 (2018)

115 S. Imajo, Y. Iwashita, K. Mishima, M. Kitaguchi, H.M. Shimizu, T. Ino,
S. Yamashita, K. Hirota, F. Goto, Y. Fuwa, R. Katayama, and NOP
Collaboration
Time-focus Experiment of Ultracold Neutron by Improved UCN
Rebuncher at J-PARC/MLF
JPS Conf. Proc. 22 011038 (2018)

105 K.M. Kojima, M. Hiraishi, A. Koda, H. Okabe, S. Takeshita, H. Li, R.
Kadono, M.M. Tanaka, M. Shoji, T. Uchida, and S.Y. Suzuki
Development of General Purpose μSR Spectrometer ARTEMIS at S1Experimental Area, MLF J-PARC
JPS Conf. Proc. 21 011062 (2018)

116 N. Oi, H.M. Shimizu, K. Hirota, M. Kitaguchi, C.C. Haddock, W.M.
Snow, T. Yoshioka, K. Mishima, T. Ino, and T. Shima
A Search for Possible Deviations from Newtonian Gravity at the nm
Length Scale Using Neutron-Noble Gas Scattering
JPS Conf. Proc. 22 011039 (2018)

106 R. Katayama, K. Mishima, S. Yamashita, M. Kitaguchi, T. Yoshioka, Y.
Seki, M. Mitsuhashi, M. Sugihara, M. Hino, E. Watanabe, D. Tsuya,
M. Saito, and N.L. Yamada
Development of new neutron mirrors for measuring the neutron
electric dipole moment
JPS Conf. Proc. 22 011009 (2018)

117 T. Kumada, K. Akutsu, K. Ohishi, T. Morikawa, Y. Kawamura, M.
Sahara, J. Suzuki, and N. Torikai
Development of Dynamic Nuclear Polarization System for SpinContrast-Variation Neutron Reflectometry
JPS Conf. Proc. 22 11015 (2018)

107 R. Maruyama, D. Yamazaki, and K. Soyama
Effect of the interfacial roughness correlation on the reflectivity in aneutron multilayer mirror
JPS Conf. Proc. 22 011011 (2018)

118 Y. Ogata, T. Abe, S. Yonemori, N.L. Yamada, D. Kawaguchi, and K.
TanakaImpact of the Solid Interface on Proton Conductivity in Nafion Thin
Films
Langmuir 34 15483–15489 (2018)

108 J.D. Parker, M. Harada, H. Hayashida, K. Hiroi, T. Kai, Y. Matsumoto,
T. Nakatani, K. Oikawa, M. Segawa, T. Shinohara, Y.H. Su, A. Takada,
T. Takemura, T. Taniguchi, T. Tanimori, and Y. Kiyanagi
Development of Energy-Resolved Neutron Imaging Detectors at

119 K. Shimokita, I. Saito, K. Yamamoto, M. Takenaka, N.L. Yamada, andT. Miyazaki
Effect of Preferential Orientation of Lamellae in Interfacial Region
between Block Copolymer-based Pressure-Sensitive Adhesive andMLF Annual Report 2018

Solid Substrate on the Peel Strength
Langmuir 34 2856–2864 (2018)
120 K. Yanagi, N.L. Yamada, K. Kato, K. Ito, and H. Yokoyama
Polyrotaxane brushes dynamically formed at a water/elastomer
interface
Langmuir 34 5297–5302 (2018)
121 F. Endo, R. Okoshi, K. Takaesu, N. Kurokawa, H. Iwase, T. Maeda,
and A. Hotta
Mechanically tough syndiotactic polypropylene (sPP) gels realized by
fast quenching using liquid nitrogen
Macromolecules 51 2321–2327 (2018)
122 Y. Shudo, A. Izumi, K. Hagita, T. Yamada, K. Shibata, and M.
Shibayama
Diffusion Behavior of Methanol Molecules Confined in Cross-linked
Phenolic Resins Studied using Neutron Scattering and Molecular
Dynamics Simulations
Macromolecules 51 6334–6343 (2018)
123 T. Iwamoto, Y. Doi, K. Kinoshita, A. Takano, Y. Takahashi, E. Kim, T.
Kim, S. Takata, M. Nagao, and Y. Matsushita
Conformations of ring polystyrenes in semidilute solutions and in
linear polymer matrices studied by SANS
Macromolecules 51 6836–6847 (2018)
124 T. Koyama, K. Ueno, M. Sekine, Y. Matsumoto, T. Kai, T. Shinohara,
H. Iikura, H. Suzuki, and M. Kanematsu
Deformation Analysis of Reinforced Concrete using Neutron Imaging
Technique
Materials Research Proceedings 4 155–160 (2018)
125 M. Kumagai, T. Uchida, K. Murasawa, M. Takamura, Y. Ikeda, H.
Suzuki, Y. Otake, T. Hama, and S. Suzuki
Convergence Behavior in Line Profile Analysis Using Convolutional
Multiple Whole-Profile Software
Materials Research Proceedings 6 57–62 (2018)
126 T.Z. Sun, A.S. Tremsin, M.J. Roy, M. Hofmann, P.B. Prangnell, and
P.J. Withers
Investigation of residual stress distribution and texture evolution in
AA7050 stationary shoulder friction stir welded joints
Materials Science & Engineering A 712 531–538 (2018)
127 Y. Sato, Y. Murakami, I. Satoshi, and N. Ishikawa
Critical Conditions of Cold Cracking in High Strength Steel Weld Basedon the Local Stress Distribution and Hydrogen Accumulation
Materials Science Forum 941 153–157 (2018)
128 K. Murasawa, M. Takamura, M. Kumagai, Y. Ikeda, H. Suzuki, Y. Otake,
T. Hama, and S. Suzuki
Determination Approach of Dislocation Density and Crystallite Size
Using a Convolutional Multiple Whole Profile Software
Materials Transactions 59 1135–1141 (2018)
129 A. Taketani, Y. Wakabayashi, Y. Otake, Y. Ikeda, T. Wakabayashi, K.
Kono, T. Kai, K. Oikawa, H. Sunaga, M. Yamada, and T. Nakayama
Quantification of localized water image in under-film corroded steel
with high spatial resolution, high time resolution, and wide view byneutron radiography
Materials Transactions 59 976–983 (2018)
130 B. Li, H. Wang, Y. Kawakita, Q. Zhang, M. Feygenson, H.L. Yu, D. Wu,
K. Ohara, T. Kikuchi, K. Shibata, T. Yamada, X.K. Ning, Y. Chen, J.Q.
He, D. Vaknin, R.Q. Wu, K. Nakajima, and M.G. Kanatzidis
Liquid-like thermal conduction in intercalated layered crystalline
solidsNature Materials 17 226–230 (2018)
131 W.L. Yao, C.Y. Li, L.C. Wang, S.J. Xue, Y. Dan, K. Iida, K. Kamazawa,
K.K. Li, C. Fang, and Y. Li

MLF Operations in 2018

Topological spin excitations in a threedimensional antiferromagnet
Nature Physics 14 1011–1015 (2018)132 T. Fujiwara, Y. Mitsuya, and H. Takahashi
Radiation imaging with glass gas electron multipliers (G-GEMs)
Nucl. Instrum. Methods Phys. Res., Sect. A 878 40–49 (2018)
133 R. Maruyama, D. Yamazaki, K. Akutsu, T. Hanashima, N. Miyata, H.
Aoki, M. Takeda, and K. Soyama
Development of high-polarization Fe/Ge neutron polarizing
supermirror: Possibility of fine-tuning of scattering length density inion beam sputtering
Nucl. Instrum. Methods Phys. Res., Sect. A 888 70–78 (2018)
134 W.H. Guan, E. Wakai, T. Naoe, H. Kogawa, T. Wakui, K. Haga, H.
Takada, and M. Futakawa
Optimization study on structural analyses for the J-PARC mercury
target vessel
Nucl. Instrum. Methods Phys. Res., Sect. A 894 8–19 (2018)
135 B. Kim, S. Bae, H. Choi, S. Choi, N. Kawamura, R. Kitamura, H. Sanko,
Y. Kondo, T. Mibe, M. Otani, G.P. Razuvaev, and E. Won
Development of a microchannel plate based beam profile monitor fora re-accelerated muon beam
Nucl. Instrum. Methods Phys. Res., Sect. A 899 22–27 (2018)
136 M. Harada, M. Teshigawara, M. Ohi, E. Klinkby, L. Zanini, K. Batkov,
K. Oikawa, Y. Toh, A. Kimura, and Y. Ikeda
Experimental validation of the brightness distribution on thesurfaces of coupled and decoupled moderators composed of 99.8%
parahydrogen at the J-PARC pulsed spallation neutron source
Nucl. Instrum. Methods Phys. Res., Sect. A 903 38–45 (2018)
137 S. Itoh, M. Nakaji, Y. Uchida, M. Kitaguchi, and H.M. Shimizu
Pendellosung interferometry by using pulsed neutrons
Nucl. Instrum. Methods Phys. Res., Sect. A 908 78 (2018)
138 M. Teshigawara, Y. Ikeda, M. Ooi, M. Harada, H. Takada, M. Kakishiro,
G. Noguchi, T. Shimada, K. Seita, D. Murashima, K. Fukatani, K.
Kanomata, and T. Teraoku
Implementation of a low-activation Au-In-Cd decoupler into the
J-PARC 1 MW short pulsed spallation neutron source
Nuclear Materials and Energy 14 14–21 (2018)
139 T. Takamuku, T. Tokuda, T. Uchida, K. Sonoda, B.A. Marekha, A. Idrissi,
O. Takahashi, Y. Horikawae, J. Matsumura, T. Tokushima, H. Sakurai,
M. Kawano, K. Sadakane, and H. Iwase
Hydrogen bonds of the imidazolium-ring of ionic liquids with DMSO
studied by NMR, soft X-ray spectroscopy, and SANS
Phys. Chem. Chem. Phys. 20 12858 (2018)
140 Y. Ishii, K. Komatsu, S. Nakano, S. Machida, T. Hattori, A. SanoFurukawa, and H. Kagi
Pressure-induced stacking disorder in boehmite
Phys. Chem. Chem. Phys. 20 16650 (2018)
141 S. Bae, H. Choi, S. Choi, Y. Fukao, K. Futatsukawa, K. Hasegawa, T.
Iijima, H. Iinuma, K. Ishida, N. Kawamura, B. Kim, R. Kitamura, H.S.
Ko, Y. Kondo, S. Li, T. Mibe, Y. Miyake, T. Morishita, Y. Nakazawa, M.
Otani, G.P. Razuvaev, N. Saito, K. Shimomura, Y. Sue, E. Won, andT. Yamazaki
First muon acceleration using a radio-frequency accelerator
Phys. Rev. Accel. Beams 21 050101 (2018)
142 H. Shishido, Y. Miki, H. Yamaguchi, Y. Iizawa, T.D. Vu, K.M. Kojima, T.
Koyama, K. Oikawa, M. Harada, S. Miyajima, M. Hidaka, T. Oku, K.
Soyama, S.Y. Suzuki, and T. IshidaHigh-Speed Neutron Imaging Using a Current-Biased Delay-Line
Detector of Kinetic InductancePhys. Rev. Applied 10 044044 (2018)
143 A.W.T. Gregg, J.N. Hendriks, C.M. Wensrich, A. Wills, A.S. Tremsin, V.

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Luzin, T. Shinohara, O. Kirstein, M.H. Meylan, and E.H. Kisi
Tomographic Reconstruction of Two-Dimensional Residual Strain
Fields from Bragg-Edge Neutron Imaging
Phys. Rev. Applied 10 064034 (2018)
144 S. Shamoto, T.U. Ito, H. Onishi, H. Yamauchi, Y. Inamura, M. Matsuura,
M. Akatsu, K. Kodama, A. Nakao, T. Moyoshi, K. Munakata, T. Ohhara,
M. Nakamura, S. Ohira-Kawamura, Y. Nemoto, and K. Shibata
Neutron scattering study of yttrium iron garnet
Phys. Rev. B 97 054429 (2018)
145 K. Horigane, M. Fujii, H. Okabe, K. Kobayashi, R. Horie, H. Ishii, Y.F.
Liao, Y. Kubozono, A. Koda, R. Kadono, and J. Akimitsu,
Magnetic phase diagram of Sr2−xLaxIrO4 synthesized by mechanicalalloying
Phys. Rev. B 97 064425 (2018)

156 H. Tamatsukuri, H. Hiraka, K. Ikeuchi, S. Iimura, Y. Muraba, M.
Nakamura, H. Sagayama, J. Yamaura, Y. Murakami, Y. Kuramoto,and H. Hosono
Gapless magnetic excitation in a heavily electron-doped
antiferromagnetic phase of LaFeAsO0.5D0.5
Phys. Rev. B 98 174415 (2018)
157 T. Moyoshi, K. Kamazawa, M. Matsuda, and M. Sato
Inelastic neutron scattering study on the electronic transition in(Pr1-yYy)1-xCaxCoO3 single crystals
Phys. Rev. B 98 205105 (2018)

146 T. Hattori
Is there a pressure-induced discontinuous volume change in liquid Cs?
Phys. Rev. B 97 100101(R) (2018)

158 T. Okudaira, S. Takada, K. Hirota, A. Kimura, M. Kitaguchi, J. Koga, K.
Nagamoto, T. Nakao A. Okada, K. Sakai, H.M. Shimizu, T. Yamamoto,and T. Yoshioka
Angular distribution of γ rays from neutron-induced compound statesof 140La
Phys. Rev. C 97 034622 (2018)

147 I. Yamauchi, M. Hiraishi, H. Okabe, S. Takeshita, A. Koda, K.M. Kojima,
R. Kadono, and H. Tanaka
Local spin structure of the α-RuCl3 honeycomb-lattice magnet
observed via muon spin rotation/relaxation
Phys. Rev. B 97 134410 (2018)

159 C.C. Haddock, N. Oi, K. Hirota, T. Ino, M. Kitaguchi, S. Matsumoto,K. Mishima, T. Shima, H.M. Shimizu, W.M. Snow, and T. Yoshioka
A Search for deviations from the inverse square law of gravity at nm
range using a pulsed neutron beam
Phys. Rev. D 97 062002 (2018)

148 S. Hayashida, O. Zaharko, N. Kurita, H. Tanaka, M. Hagihala, M. Soda,
S. Itoh, Y. Uwatoko, and T. Masuda
Pressure-induced quantum phase transition in the quantum
antiferromagnet CsFeCl3
Phys. Rev. B 97 140405(R) (2018)

160 R. Inoue, T. Kanaya, T. Yamada, K. Shibata, and K. Fukao
Experimental investigation of the glass transition of polystyrene thinfilms in a broad frequency range
Phys. Rev. E 97 012501 (2018)

149 T. Kim, J.C. Leiner, K. Park, J. Oh, H. Sim, K. Iida, K. Kamazawa, andJ.-G. Park
Renormalization of spin excitations in hexagonal HoMnO3 bymagnon-phonon coupling
Phys. Rev. B 97 201113(R) (2018)
150 N. Murai, K. Suzuki, S. Ideta, M. Nakajima, K. Tanaka, H. Ikeda, and
R. Kajimoto
Effect of electron correlations on spin excitation bandwidth in
Ba0.75K0.25Fe2As2 as seen via time-of-flight inelastic neutron scattering
Phys. Rev. B 97 241112(R) (2018)
151 T. Nakajima, Y. Inamura, T. Ito, K. Ohishi, H. Oike, F. Kagawa, A.
Kikkawa, Y. Taguchi, K. Kakurai, Y. Tokura, and T. Arima
Phase-transition kinetics of magnetic skyrmions investidated bystroboscopic small-angle neutron scattering
Phys. Rev. B 98 014424 (2018)
152 H. Okabe, M. Hiraishi, S. Takeshita, A. Koda, K.M. Kojima, and R.
KadonoLocal electronic structure of interstitial hydrogen in iron disulfide
Phys. Rev. B 98 075210 (2018)
153 P. Wu, B. Zhang, K.L. Peng, M. Hagihala, Y. Ishikawa, M. Kofu, S.H.
Lee, H. Kumigashira, C.S. Hu, Z.M. Qi, K. Nakajima, G.Y. Wang, Z.
Sun, and T. Kamiyama
Investigation of the electronic structure and lattice dynamics of thethermoelectric material Na-doped SnSe
Phys. Rev. B 98 094305 (2018)
154 S. Lee, M.-C. Lee, Y. Ishikawa, P. Miao, S. Torii, C.J. Won, K.D. Lee, N.
Hur, D.-Y. Cho, and T. Kamiyama
Magnetoelastic octahedral breathing mode in the ferrimagnetic
La2CoIrO6 double perovskite
Phys. Rev. B 98 104409 (2018)
155 S. Torigoe, T. Hattori, K. Kodama, T. Honda, H. Sagayama, K. Ikeda, T.
Otomo, H. Nitani, H. Abe, H. Murakawa, H. Sakai, and N. Hanasaki
Nanoscale ice-type structural fluctuation in spinel titanates

172

Phys. Rev. B 98 134443 (2018)

161 T. Xie, D.L. Gong, H. Ghosh, A. Ghosh, M. Soda, T. Masuda, S. Itoh, F.
Bourdarot, L.-P. Regnault, S. Danilkin, S.L. Li, and H.Q. Luo
Neutron Spin Resonance in the 112-Type Iron-Based Superconductor
Phys. Rev. Lett. 120 137001 (2018)
162 T. Xie, Y. Wei, D.L. Gong, T. Fennell, U. Stuhr, R. Kajimoto, K. Ikeuchi,
S.L. Li, J.P. Hu, and H.Q. Luo
Odd and Even Modes of Neutron Spin Resonance in the Bilayer IronBased Superconductor CaKFe4As4
Phys. Rev. Lett. 120 267003 (2018)
163 K. Kurashima, T. Adachi, K.M. Suzuki, Y. Fukunaga, T. Kawamata, T.
Noji, H. Miyasaka, I. Watanabe, M. Miyazaki, A. Koda, R. Kadono,
and Y. Koike
Development of Ferromagnetic Fluctuations in Heavily Overdoped(Bi,Pb)2Sr2CuO6+δ Copper Oxides
Phys. Rev. Lett. 121 057002 (2018)
164 J. Sugiyama, I. Umegaki, H. Nozaki, W. Higemoto, K. Hamada, S.
Takeshita, A. Koda, K. Shimomura, K. Ninomiya, and M.K. Kubo
Nuclear magnetic field in solids detected with negative-muon spinrotation and relaxation
Phys. Rev. Lett. 121 087202 (2018)
165 Y. Sakaguchi, T. Hanashima, H. Aoki, H. Asaoka, A.-A.A. Simon, and
M. Mitkova
Kinetics of Silver Photodiffusion Into Amorphous Ge20S80 Films: Caseof Pre-Reaction
Phys. Status Solidi A 215 1800049 (2018)
166 K. Ohoyama and K. Hayashi
White Neutron Holography in Pulsed Neutron Facilities
Phys. Status Solidi B 255 1800143 (2018)
167 D. Ueta, T. Kobuke, M. Yoshida, H. Yoshizawa, Y. Ikeda, S. Itoh, andT. Yokoo
Crystalline electric field level scheme of the non-centrosymmetric
CePtSi3
Physica B 536 21–23 (2018)

MLF Annual Report 2018

168 M. Yoshida, D. Ueta, Y. Ikeda, T. Yokoo, S. Itoh, and H. Yoshizawa
Magnetic and thermodynamic studies on the charge and spin orderingin the highly hole-doped La2-xSrxCoO4
Physica B 536 338–341 (2018)
169 K. Matsuura, H. Sagayama, A. Uehara, Y. Nii, R. Kajimoto, K.
Kamazawa, K. Ikeuchi, S. Ji, N. Abe, and T. Arima
Magnetic excitations in the orbital disordered phase of MnV2O4
Physica B 536 372–376 (2018)
170 K. Ikeuchi, T. Kikuchi, K. Nakajima, R. Kajimoto, S. Wakimoto, andM. Fujita
Detailed study of the structure of the low-energy magnetic excitations
in overdoped La1.75Sr0.25CuO4
Physica B 536 717–719 (2018)

MLF Operations in 2018

Ohira-Kawamura, Y. Sakaguchi, H. Shimakura, R. Takahashi, and
K. Nakajima
Anomaly of structural relaxation in complex liquid metal of bismuth- Dynamic correlation function of coherent quasi-elastic neutron
scattering Physica B 551 291–296 (2018)
182 M. Nakamura, T. Kikuchi, K. Kamazawa, and Y. Kawakita
Phonon dynamics of NaI investigated by G(r, E) analysis
Physica B 551 351–354 (2018)
183 K. Iwasa, T. Onimaru, T. Takabatake, R. Higashinaka, Y. Aoki, S. OhiraKawamura, and K. Nakajima
Inelastic neutron scattering study on 4 f -electron multipole system
PrTr2X20 (Tr : transition metal, X : Al and Zn)
Physica B 551 37–40 (2018)

171 Z.J. Tan, P. Miao, X.H. Lin, S. Lee, Y. Ishikawa, M. Hagihala, S. Torii, Y.X.
Wang, M. Yonemura, and T. Kamiyama
The investigation of magnetic phase transition in cobaltite perovskites
byhigh-resolution neutron powder diffraction under 14 T magnetic
ﬁeld
Physica B 551 111–114 (2018)

184 W.R. Puspita, H. Takeya, T. Mochiku, Y. Ishikawa, S. Lee, S. Torii, M.
Yonemura, and T. Kamiyama
Temperature Dependence of Structural Disorder in Thermoelectric
Clathrate Ba8Al16Ge30
Physica B 551 41–45 (2018)

172 K. Nakajima and R. Kajimoto
High-energy magnetic excitations in lightly oxygen-doped lanthanum
nickel oxides
Physica B 551 142–145 (2018)

185 K. Sakurai, M. Mizusawa, J. Jiang, and T. Ito
Hadamard coding of time-of-flight neutron reflectogram at grazing
incidence
Physica B 551 426–430 (2018)

173 K. Hiroi, T. Shinohara, H. Hayashida, J.D. Parker, Y.H. Su, K. Oikawa,T. Kai, and Y. Kiyanagi
Study of the magnetization distribution in a grain-oriented magnetic
steel using pulsed polarized neutron imaging
Physica B 551 146–151 (2018)

186 K. Oikawa, Y.H. Su, R. Kiyanagi, T. Kawasaki, T. Shinohara, T. Kai, K.
Hiroi, S. Harjo, J.D. Parker, Y. Matsumoto, H. Hayashida, S.Y. Zhang,
Y. Tomota, and H. Sato
Recent progress on practical materials study by Bragg edge imaging
at J-PARC
Physica B 551 436–442 (2018)

174 M. Hirai, S. Ajito, M. Sugiyama, H. Iwase, S. Takata, N. Shimizu, N.
Igarashi, A. Martel, and L. Porcar
Macromolecular crowding effect on protein structure and hydration
clarified by using X-ray and neutron scattering
Physica B 551 212–217 (2018)
175 S. Itoh, T. Hawai, S. Ibuka, T. Yokoo, and Y. Endoh
Magnetic excitations in metallic antiferromagnets Fe0.5Mn0.5 andFe0.7Mn0.3
Physica B 551 21–23 (2018)
176 N.L. Yamada, M. Sferrazza, and S. Fujinami
In-situ measurement of phospholipid nanodisk adhesion on a solid
substrate using neutron reflectometry and atomic force microscopy
Physica B 551 222–226 (2018)
177 S. Ajito, M. Hirai, H. Iwase, N. Shimizu, N. Igarashi, and N. Ohta
Protective action of trehalose and glucose on protein hydration shell
clarified by using X-ray and neutron scattering
Physica B 551 249–255 (2018)
178 K. Akutsu, M. Cagnes, T. Niizeki, Y. Hasegawa, and T.A. Darwish
Penetration behavior of an ionic liquid in thin-layer silica coating: Ionic
liquid deuteration and neutron reflectivity analysis
Physica B 551 262–265 (2018)
179 M. Mizusawa, K. Sakurai, D. Yamazaki, and M. Takeda
An electrochemical cell with vertical geometry for neutron reflectivity
measurements
Physica B 551 270–273 (2018)
180 J. Abe, K. Sekine, S. Harjo, T. Kawasaki, and K. Aizawa
Effect of gauge volume on strain measurement in rock materials using
time-of-flight neutron diffraction
Physica B 551 283–286 (2018)
181 Y. Kawakita, T. Kikuchi, Y. Inamura, S. Tahara, K. Maruyama, T.
Hanashima, M. Nakamura, R. Kiyanagi, Y. Yamauchi, K. Chiba, S.

187 N. Miyata and T. Miyazaki
Relatively thick (few micrometers) film structure estimated by backincidence neutron reflectometry
Physica B 551 449–451 (2018)
188 Y. Ishikawa, J.R. Zhang, R. Kiyanagi, M. Yonemura, T. Matsukawa, A.
Hoshikawa, T. Ishigaki, S. Torii, R. Oishi-Tomiyasu, and T. Kamiyama
Z-MEM, Maximum Entropy Method software for electron/nuclear
densitydistribution in Z-Code
Physica B 551 472–475 (2018)
189 M. Nakamura, W. Kambara, K. Iida, R. Kajimoto, K. Kamazawa, K.
Ikeuchi, M. Ishikado, and K. Aoyama
Performances of oscillating radial collimator for the Fermi chopper
spectrometer 4SEASONS at J-PARC
Physica B 551 480–483 (2018)
190 T. Kai, S. Sato, K. Hiroi, Y.H. Su, M. Segawa, J.D. Parker, Y. Matsumoto,
H. Hayashida, T. Shinohara, K. Oikawa, and Y. Kiyanagi
Characteristics of the 2012 model lithium-6 time-analyzer neutron
detector (LiTA12) system as a high efficiency detector for resonanceabsorption imaging
Physica B 551 496–500 (2018)
191 H. Iwase, S. Takata, T. Morikawa, M. Katagiri, A. Birumachi, and J.
Suzuki
Installation of a high-resolution position-sensitive scintillation
detector in the small and wide angle neutron scattering instrument(TAIKAN), MLF, J-PARC
Physica B 551 501–505 (2018)
192 Y. Seki, T. Shinohara, W. Ueno, J.D. Parker, and Y. Matsumoto
Effect of upstream beam collimation on neutron phase imaging witha Talbot-Lau interferometer at the RADEN beam line in J-PARC
Physica B 551 512–516 (2018)
193 P. Wu, Y. Ishikawa, M. Hagihala, S. Lee, K.L. Peng, G.Y. Wang, S. Torii,

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and T. Kamiyama
Crystal structure of high-performance thermoelectric materials byhigh resolution neutron powder diffraction
Physica B 551 64–68 (2018)
194 S. Lee, S. Torii, Y. Ishikawa, M. Yonemura, T. Moyoshi, and T.
Kamiyama
Weak-ferromagnetism of CoF3 and FeF3
Physica B 551 94–97 (2018)
195 S. SatohDevelopment of a Flat-Panel and Resistor-Type Photomultiplier Tube
System for High Position-Resolution Two-Dimensional Neutron
Detector
Plasma and Fusion Research 13 2405056 (2018)
196 F.A. Mavuso, N.V. Mdlovu, K.-S. Lin, K. Ohishi, K. Dehvari, N.B.
Mdlovu, and Y.-S. Lin
Synthesis and structural characterization of polymer-magnetic
nanocomposites as carriers for drug delivery system
Proc. of 450th International Conference on Recent Advances in
Medical Science (ICRAMS) (2018)
197 K. Moriyama, T. Nakatani, Y. Yasu, H. Ohshita, and T. Seya
Development of status analysis system based on ELK stack at J-PARC
MLF
Proceedings of 16th Int. Conf. on Accelerator and Large
Experimental Control Systems 1423–1427 (2018)
198 T. Kumada, K. Akutsu, K. Ohishi, Y. Kawamura, T. Morikawa, M.
Sahara, J. Suzuki, and N. Torikai
Development of closed-cycle dynamic nuclear polarization system forsmall-angle neutron scattering and neutron reflectometry
Proceedings of Science 324 9 (2018)
199 K. Akutsu, M. Sahara, T. Niizeki, S. Suzuki, Y. Hasegawa, M. Yoshii, A.
Shimomura, and H. Komatsuzaki
Development of new waterproof thin-layers for the magnetic alloy
core and structural study by neutron reflectometry
Proceedings of the 15th Annual Meeting of Particle Accelerator
Society of Japan 1198–1201 (2018)
200 Y. Nakamura, A. Shibata, W. Gong, S. Harjo, T. Kawasaki, A. Ito, and
N. Tsuji
In Situ Neutron Diffraction Study on Microstructure Evolution During
Thermo-Mechanical Processing of Medium Manganese SteelProceedings of the International Conference on Martensitic
Transformations: Chicago 155–158 (2018)
201 N. Tsuchida and S. Harjo
TRIP Effect in a Constant Load Creep Test at Room Temperature
Proceedings of the International Conference on Martensitic
Transformations: Chicago 43–46 (2018)
202 N. Kawamura, M. Aoki, J. Doornbos, T. Mibe, Y. Miyake, F. Morimoto,Y. Nakatsugawa, M. Otani, N. Saito, Y. Seiya, K. Shimomura, A.
Toyoda, and T. Yamazaki
New concept for a large-acceptance general-purpose muon beamline
Progress of Theoretical and Experimental Physics 2018 113G01(2018)
203 A. Sano-Furukawa, T. Hattori, K. Komatsu, H. Kagi, T. Nagai, J.J.
Molaison, A.M. dos Santos, and C.A. Tulk
Direct observation of symmetrization of hydrogen bond in δ-AlOOH
under mantle conditions using neutron diffraction
Scientific Reports 8 15520 (2018)
204 M. Ishikado, S. Shamoto, K. Kodama, R. Kajimoto, M. Nakamura, T.
Hong, and H. Mutka
High-energy spin fluctuation in low-Tc iron-based superconductor
LaFePO0.9
Scientific Reports 8 16343 (2018)174

205 M. Sales, M. Strobl, T. Shinohara, A. Tremsin, L.T. Kuhn, W.R.B.
Lionheart, N.M. Desai, A.B. Dahl, and S. Schmidt
Three Dimensional Polarimetric Neutron Tomography of Magnetic
FieldsScientific Reports 8 2214 (2018)
206 V. Ukleev, S. Suturin, T. Nakajima, T.-H. Arima, T. Saerbeck, T.
Hanashima, A. Sitnikova, D. Kirilenko, N. Yakovlev, and N. Sokolov
Unveiling structural, chemical and magnetic interfacial peculiaritiesin ε-Fe2O3/GaN (0001) epitaxial films
Scientific Reports 8 8741 (2018)
207 R. Kajimoto, M. Nakamura, N. Murai, S. Shamoto, T. Honda, K. Ikeda,
T. Otomo, H. Hata, T. Eto, M. Noda, H. Kuwahara, and T. Okuda
Elastic and dynamical structural properties of La and Mn-doped
SrTiO3 studied by neutron scattering and their relation with thermal
conductivities
Scientific Reports 8 9651 (2018)
208 K. Kataoka, H. Nagata, and J. Akimoto
Lithium-ion conducting oxide single crystal as solid electrolyte foradvanced lithium battery application
Scientific Reports 8 9965 (2018)
209 B. Wang, H.Y. He, M. Naeem, S. Lan, S. Harjo, T. Kawasaki, Y.X. Nie,
H.W. Kui, T. Ungár, D. Ma, A.D. Stoica, Q. Li, Y.B. Ke, C.T. Liu, and X.L.
Wang
Deformation of CoCrFeNi high entropy alloy at large strain
Scripta Materialia 155 54–57 (2018)
210 J.-J. Kang, T.-Y. Yang, Y.-K. Lan, W.-R. Wu, C.-J. Su, S.-C. Weng, N.L.
Yamada, A.-C. Su, and U.-S. Jeng
Directed Vertical Diffusion of Photovoltaic Active Layer Components
into Porous ZnO-based Cathode Buffer Layers
Small 14 1704310 (2018)
211 H. Tanoue, K. Inoue, N.L. Yamada, K. Kohzo, S. Miyao, T. Ishizone,
and H. Yokoyama
Thermoresponsive Dynamic Polymer Brush Fabricated by the
Segregation of Amphiphilic Diblock Copolymers
Soft matter 14 5930–5935 (2018)
212 N. Ishida, K. Miyazawa, N. Kitamura, J. Akimoto, and Y. Idemoto
Average and local structure analysis of metastable LixMn0.9Ti0.1O2 bysynchrotron X-ray and neutron sources
Solid State Ionics 325 209–213 (2018)

MLF Annual Report 2018

Editorial Board

Editorial Board - MLF Annual Report 2018

Chief Editor

Yuhua SuTechnology Development Section

Tazuko Mizusawa
CROSS

Jun AbeYukinori Nagatani

Akinori Hoshikawa

Takashi Naoe

Kazutaka Ikeda

Kenichi Oikawa

Yoshihisa Ishikawa

Kaoru Sakasai

CROSS

Ibaraki University

Neutron Science Section

CROSS

Muon Science Section

Neutron Source Section

Neutron Science Section

Neutron Instrumentation Section

Yukiko Nagai

Technology Development Section

175J-PARCHigh Energy Accelerator Research Organization (KEK)
Japan Atomic Energy Agency (JAEA)

J-PARC ANNUAL REPORT 2018

Japan Proton Accelerator Research Complex

Vol.2: Materials and Life Science Experimental Facility

http://j-parc.jp/
Materials and Life Science Division
J-PARC Center

https://mlfinfo.jp/enhttps://neutron.cross.or.jp/en

J-PARC 19-02

J-PARC Center

Comprehensive Research Organization for Science and Society