MLF Annual Report 2013

MLF
ANNUAL REPORT
2013

J-PARC 14-03
KEK Progress Report 2014-4

Materials and Life Science Division
J-PARC Center

Tokai, Naka-gun, Ibaraki 319-1195, Japan

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

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

Preface to the MLF Annual Report 2013

After the recovery from the disaster, which occurred in 2011, the facility had been operating quite steadily
with a fairly high power at 200 kW and then 300 kW, starting from January 2012. However, an incident in the
Hadron Facility, one of the three facilities in J-PARC, occurred at midnight on May 23, 2013. This incident
forced the shutdown of the whole facility of J-PARC. J-PARC staffs made significant efforts and spent a longtime to make assessment of the root cause of the incident, safety analysis, revision of the safety system/
organization/manuals, safety drills, explanations to the local public and both the local and the central
governments. Then finally we, MLF, were able to obtain an approval for resuming the operation of the facility
in January 2014. The user program was seriously affected by the unexpected long shutdown, and morethan half of the scheduled experiments for the 2013A term were canceled without any compensation. Here,I sincerely apologize to the MLF users for this incidence and hope to regain sustainable support and mutual
reliance.
During the shutdown, we improved the target system and the helium bubbling system, by modifying a partof the mercury (Hg) cooling loop, and realized a full injection of helium bubbles into the Hg flaw. We foundout that, during the operation in 2013, the vibration caused by the cavitation in the Hg-target on the proton
bombardment had been drastically reduced, which may mitigate significantly the pitting damage on the target
container.
When we called for proposals for 2013B in October 2013, we received a large number of applications.
Although the operation time for the user program was very limited, we found a large over-subscription. We
were impressed by the high expectations from our facility, and confirmed our responsibility to provide astable operation to the users. Since then the number of applications is steadily increasing, accompanied by asteady increase of users. As of September 2014, the number of general proposals and that of unique users
exceeded 750 and 1000 respectively. We are now preparing to ramp up the accelerator power to more than
500 kW in late November 2014. The MLF facility is now almost ready to become a world class user facility inthe very near future.

Masatoshi Arai
Division Head of Materials and Life Science Division (MLF)Three years have passed since CROSS-Tokai commenced operations in support of the user program on the
Public Beamlines at the Materials and Life Science Experimental Facility of J-PARC (J-PARC MLF).
As required by the “Promotion of Public Utilization of Specific Advanced Large-scale Research Facilities”
legislation, under which CROSS was appointed and operates, we are now fully engaged in facility promotion
activities such as operating a fair and open proposal selection system for the MLF Public Beamlines, the provisionof high-quality user support and the promotion of facility utilization by both academic and industrial researchers.
During 2013, CROSS-Tokai supported the user program on six fully-operational Public Beamlines: BL01
4SEASONS, BL02 DNA, BL11 PLANET, BL15 TAIKAN, BL17 SHARAKU and BL18 SENJU. In addition, construction
work continued on the seventh Public Beamline, BL22 RADEN, which will be available to users in 2015. Unfortunately,user operations during the year were severely affected by the Hadron Facility incident and its aftereffects with
beamtime being available during April-May 2013 and from mid-February to the end of March 2014 only.
A further important responsibility of CROSS-Tokai is the evaluation of Contract Beamlines at the MLF. During 2013,
the Contract Beamline Evaluation Committee established by CROSS-Tokai during 2012, undertook and completed
reviews of the operation and performance of the two Ibaraki Prefecture beamlines: BL03 iBIX and BL20 iMATERIA.
Special programs to promote facility utilization developed by CROSS-Tokai in 2012, continued to operate
successfully during 2013 and a summary of these activities is presented in this Report. These include:•

Trial Use – a program that promotes the use of neutrons by first-time or novice users from both theindustrial and academic sectors;•

Elements Strategy Initiative – an integrated strategic research program of the Japanese governmentthat aims to promote the development of innovative materials and alternative technologies in the target
areas of permanent magnets, catalysis and batteries, and electronic and structural materials; and,•Complementary Use – a program designed to encourage and facilitate the complementary andcollaborative use of pulsed neutrons (J-PARC MLF) and synchrotron radiation (SPring-8).

In the area of facility utilization promotion, we have in the last year joined with JASRI – our sister organization
at SPring-8 – to develop a system of Complementary Use proposals. This system aims to encourage and facilitate
complementary and collaborative use of multiple large-scale facilities – initially neutron and synchrotron radiation
sources – in a single research project. We hope that, ultimately, the system will develop to a stage where users
can make a single research proposal to multiple facilities.
I hope that this Annual Report will be a useful resource for anyone wishing to know more about the current
status of the MLF, the recent scientific outcomes, the technical R&D projects that support the science program, andthe operational details of our facility.
On behalf of the team at CROSS-Tokai, I extend a warm welcome to all researchers who wish to make use of
the Public Beamlines at J-PARC MLF.

Hideaki Yokomizo
Director, CROSS-Tokai* Research Center for Neutron Science and Technology, Comprehensive Research Organization for Science and Society
www.cross-tokai.jp

Contents
Preface to the MLF Annual Report 2013

Research and Development Highlights
Investigations of 3D Atomic Local Structures around Dopants
by Neutron Atomic Resolution Holography·············································································

2

Magnetic Frustration in 5d Iridium Spinel CuIr2S4 Investigated by Muon Spin Relaxation······················

5

SuperHRPD Finds Tiny Ru-O Bond Increments as Small as 0.0005 Å
in Itinerant Ferromagnetic SrRuO3························································································

7

Visualization of Magnetic Field Distribution
by Polarized Pulsed Neutron Imaging Inside the Power Magnetic Instruments······························

9

Detection of High Elastic Strain in Fe3Pt Using TAKUMI································································ 11
Strengthening Mechanism of Advanced Steel with Deformation Induced Phase Transformation············ 13
Diffraction Study of High Neutron Absorbing Material EuGa4 on SENJU··········································· 15
Crystal Structures and Hydrogen Bonding in High-pressure and High-temperature Phasesof Ca(OD)2······················································································································ 17
Neutron Crystal Structure Analysis of Human α-Thrombin-Inhibitor Complex using iBIX······················ 19
Neutron Diffraction Study for Reaction Mechanism of RNase A by using iBIX···································· 21
Local Structural Changes with Amorphization on Thermal Decomposition Reaction of LiAl(ND2)4·········· 23
Polymer Brush Layers at Water/Polymer Interfaces Formed by Segregationof Amphiphilic Block Copolymers························································································· 25
Multistep Thickening of Nafion Thin Films in Water Studied by Optical and Neutron Reflectivity············ 27
Precise Evaluation of Angstrom-Ordered Mixed Interfaces in Solution Processed OLEDs:
Influence on Carrier Transport Characteristics········································································ 29
SANS and SAXS Studies on Aggregates Properties of a Novel Sugar-Type Surfactant
in Aqueous Solution·········································································································· 31
Neutron Brillouin Scattering of Hydrated β-Lactoglobulin······························································· 33
Inelastic Neutron Scattering Study in Multiferroic Compound NdFe3(11BO3)4······································ 35
Spin-Wave Dispersion in Nd-Fe-B Permanent Magnets Observed by Neutron Brillouin Scattering········· 37
Doping-Evolution of High-Energy Spin Excitation in the Electron-Doped Pr1.4−xLa0.6CexCuO4················· 39
Multiple-Probe Study of Highly Hydrogen Doped Fe-based superconductor LaFeAsO1-xHx··················· 41
Long Periodic Chiral Helimagnetic Ordering in T1/3MS2 (T = Transition Metal, M = Nb and Ta)··············· 43
Detailed Study of the Phase Diagram of Fe-Based Superconductor Ba(Fe1-xCox)2As2·························· 45
Electrical Activity of Interstitial Hydrogen in BaTiO3 Simulated with Positive Muons····························· 47
Synthesis, Structure, and Conduction Mechanismof the Lithium Superionic Conductor Li10+δGe1+δP2-δS12······························································· 49
Development on Non-Destructive Elemental Analysis
for Extraterrestrial Materials using a Muon Beam···································································· 51
Superconducting Nanowire Neutron Detector············································································· 54

Neutron Source
Progress of the Neutron Source Section···················································································· 58
Status of Proton Beam Commissioning of MLF··········································································· 60

Improvement of Pressure Wave Mitigation Function in Mercury Target System································· 62
Cryogenic Hydrogen System··································································································· 64
Modification of the MLF General Control System for Sustainable Long-Term Operation······················· 66
Scenes from the Neutron Target Station···················································································· 68

Neutron Science
Neutron Science··················································································································· 70
BL01: 4D-Space Access Neutron Spectrometer 4SEASONS························································· 73
BL02: TOF type Si Crystal Analyzer near Backscattering Spectrometer DNA- Specification and Commissioning Results -·········································································· 75
Current Status of IBARAKI Biological Crystal Diffractometer iBIX at BL03········································· 77
Study of the Energy Resolution of the Pulsed Neutron Beam Provided by ANNRI (BL04)···················· 79
Studies of Neutron Optics for Physics Researches······································································ 83
Advance Neutron Beam Line
for VIllage of Neutron ResOnance Spin Echo Spectrometers (VIN ROSE) at BL06························ 85
Upgrade of SuperHRPD········································································································· 87
Development of an Advanced Special Neutron Powder Diffractometer
under Extreme Environment for Materials·············································································· 89
BL10: NOBORU··················································································································· 91
BL11: High-Pressure Neutron Beamline PLANET Opened for General Users···································· 93
High Resolution Chopper Spectrometer at BL12········································································· 96
BL14 AMATERAS················································································································· 98
Upgrading of TAIKAN and Needs of the Users············································································ 100
Development of Sample Environments of SOFIA Reflectometer
for Seconds-Order Time Slicing Measurement········································································ 102
BL17 Polarized Neutron Reflectometer, SHARAKU······································································ 104
BL18: Current Status of SENJU······························································································· 106
Engineering Studies at BL19-TAKUMI······················································································· 108
Current Status of the Versatile Neutron Diffractometer, iMATERIA··················································· 111
Status of the High Intensity Total Diffractometer (BL21, NOVA)······················································· 113
BL22: Construction of Energy-resolved Neutron Imaging System “RADEN”······································ 115
Recent Progress on Polarized Inelastic Neutron Spectrometer POLANO·········································· 117
Performance of Spin Devices for Polarized Neutrons of POLANO··················································· 120
Status of Instrumentation for Dynamic Nuclear Polarization of Proton Spins······································ 122
Development of a Compact in-situ SEOP 3He Neutron Spin Filter··················································· 124
Sample Environment at MLF··································································································· 126
IROHA Upgrade··················································································································· 128
A Scintillator-Based Detector with Sub 100-µm Spatial Resolution for Time-of-Flight Neutron Imaging···· 130
Two-Dimensional Multiwire Neutron Detector with Individual Line Readout
and Optical Signal Transmission·························································································· 132
Study on the In-plane Magnetic Structure of the Neutron Polarizing Multilayer Mirror·························· 133
Scenes from the Neutron Experimental Hall··············································································· 135

Muon Science
Status of J-PARC MUSE········································································································ 138
Development of the Muon Production Target at MUSE································································· 140
Present Status of the D-Line··································································································· 143
Present Status of the U-Line··································································································· 147
Construction of the S-Line······································································································ 151
Present Status of the H-Line··································································································· 153
Scenes from the Muon Experimental Hall·················································································· 156

Radiation Safety
Radiation Safety··················································································································· 158
Scenes from the Emergency drill······························································································ 161

Whatʼs new at the MLF in 2013?
Activities of the Technology Development Section······································································· 164

MLF Operations in 2013
CROSS-Tokai - 2013 Update·································································································· 168
Beam Operation Status at MLF································································································ 174
Users at the MLF·················································································································· 175
Proposal Review System········································································································ 176
MLF Proposals Summary – FY2013························································································· 177
MLF Division Staff 2013········································································································· 180
CROSS-Tokai Staff 2013········································································································ 183
Committees and Meetings······································································································ 185
Workshops in 2013··············································································································· 193
Seminars and Courses in 2013································································································ 199
Schools in 2013···················································································································· 200
Award List··························································································································· 201
MLF Publication 2013············································································································ 202
Editorial Board - MLF Annual Report 2013················································································· 209

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

Organizaon Chart ofCROSS

Deputy Director (JAEA, KEK, Safety)

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

Safety Division

President

Accelerator Division

Materials & Life Science Division
Neutron Source Secon
Neutron Science Secon
Neutron InstrumentaonSeconMuon Science SeconTechnology Development
SeconCROSS Head Office
Research center for
Science and Society

Director,
CROSS-Tokai
Science Coordinators
Safety Division
Administraon DivisionUlizaon Promoon
Division
Neutron R&D DivisionParcle & Nuclear Physics Division
Transmutaon Secon
Cryogenics Secon
Operaons Support SeconInformaon System Secon
Public Relaons Secon

The Role of CROSS-Tokai
Under the terms of the legislation that supports
the Public Neutron Beam Facility, CROSS-Tokai is
entrusted with specific responsibilities. In practicalterms, the core functions of CROSS-Tokai can besummarized as follows:	Proposal Selection and Beamtime Allocation on
the Public Beamlines	User Support on the Public Beamlines

Administraon Division
Users Office Team	Establishment of an Information Resource for
Facility Users
	Outreach and Facility Utilization Promotion
	Contract Beamline Assessment and Selection

J-PARC MAPCROSS-Tokai(Ibaraki Quantum Beam Research Center)

R245

J-PARC Center Users Office(

KEK-Tokai

Linac

Main Gate
R245

HENDEL R&D Building

3 GeV Synchrotron

MLF

50 GeV Synchrotron

Research and Development
Highlights

Investigations of 3D Atomic Local Structures around Dopants
by Neutron Atomic Resolution Holography

Topical Results

1. Introduction
The performance of most of functional materials can be controlled by doping; for instance, theelectrical conductivity of silicon can be controlled
by doping a very small amount of boron or phosphorus. Thus, understanding the distortions of local
atomic structures around the dopants from the average structures is indispensable to clarify the mechanisms of functionability. Recently, pair distributionfunction (PDF) method, and X-ray absorption finestructure (XAFS) method are actively used for local
structure investigations. However, these methods
provide only information on the distance between atoms, and cannot observe 3D structures. Moreover,even for radiation X-rays, accurate observations oflight elements, such as B, Li, H, in materials are difficult in spite of the importance of those elements.
The authors are developing the neutron atomic
resolution holography (ARH) for investigations oflocal structures of light elements in materials. The
ARH is the unique probe to observe 3D local atomic
structures using interference between a wave, whichis scattered by elements (object wave), and a wave,
which is not scattered (reference wave) [1,2]. The
detailed principles can be found in Ref.2. The advantages of ARH in comparison with other methods

are as follows: (a) 3D atomic images can be visualized without models. (b) 3D local structures within~20 Å around a dopant can be observed. (c) the
center element can be selected. Photoelectron andfluorescent X-rays ARH have been already in practical use for materials science in Japan. However,light elements cannot be observed accurately byelectrons or X-rays. To overcome this, Cser et al.
proposed the neutron ARH in 2001 [3], and the first
demonstration experiment was performed using asingle crystal of Al4Ta3O13(OH) by Sur et al. in ChalkRiver Laboratory, Canada [4]. However, the neutron
ARH is still in the demonstration stage. Thus, we
aim at developing a neutron ARH for practical investigations in materials science.
2. Neutron ARH experiments
There are two types of neutron ARH experiments: normal method and inverse method [2]. The
important difference is that the neutron intensity ismeasured for the normal method, while the intensity of prompt g-ray is measured for inverse method.
For experiments on BL10, the inverse method wasused. The principle of the normal method can befound in Ref. 2 and 5, and is not explained here.
Figure 1 shows the principle of the inverse

Figure 1. Principle of neutron ARH for the inverse method (from Ref.1).

2

Research and Development Highlights



(1)

where b is a scattering length of the nuclear, l iswavelength of neutrons, d is the distance between
elements A and B. Transformations from the holograms to atomic images can be found in Ref. 2.
We already performed the normal method neutron
ARH experiments of a PdH0.78 single crystal in JRR-3
of Japan Atomic Energy Agency, and succeeded invisualizing the atomic structure around a hydrogen[5]. However, the accuracy of the atomic image was
not sufficient because of fake images (the so-called
twin images). The main reason for the poor accuracy was that only the monochromatic beam with l= 1.82 Å was used in the experiments; to avoid twin

λ=0.42Å

images, measurements using many wavelengths
are effective. However, multi-wavelength experiments in reactor facilities require impracticably longmeasurement times. To overcome this, we are developing a novel technique, the pulsed neutron ARH
by the inverse method. Since pulsed neutrons arewhite beams, a large number of holograms with different wavelengths can be obtained at once. Thus,
we expect that pulsed neutron ARH can enhancedrastically the accuracy of atomic images.

Topical Results

method. The reference wave is the incident neutron
beam as plane wave, and the object wave is spherical wave scattered by the element B. The interference between the reference and object wave generates standing wave in the sample; the intensity ofthe standing wave is dependent on the positional
relation between elements A and B, and the direction of the incident beam. When element A has alarge absorption cross-section, such as for B, g-ray
is generated isotropically by the absorption at element A. Since the intensity of the g-ray is proportional to the amplitude of the standing wave at element A, the intensity map gives us information oninterference, that is, a hologram. A hologram can be
represented as follows:

3. Results of Neutron ARH on BL10
In 2013, we performed the world’s first pulsed
neutron ARH experiments on BL10 at J-PARC by
the inverse method, and obtained about 120 holograms with different wavelengths. The instrument
consists of a g-ray counter with Pb shield and a f-w
goniometer. The intensity of the g-ray was observedby the event recording method during continuous
move of the goniometer. The sample was a single
crystal of 1% Eu doped CaF2, which is an important material for neutron scintillation counters under high temperature and humidity. Figure 2 shows
typical holograms that have angular dependence on
the intensity of the g-ray from the sample. Since Eu
has a large absorption cross section (4530 b at l =1.80 A), and those of Ca and F are relatively negligible, it means that the observed g-ray was caused
from the doped Eu; thus, the obtained holograms
show the local structure around doped Eu.

λ=2.21ÅFigure 2. Obtained holograms on BL10 with wavelength of 0.42 Å and 2.21 Å. The red arrows show standing wave lines.

Research and Development Highlights

3

Topical Results

Some of the obtained holograms clearly show
linear structures called standing wave lines (red arrows in Fig.2); the lines in Fig.2 indicate the direction of (001) axes around Eu. These standing wave
lines definitely mean that we succeeded in observing the symmetry of the local structure around Eu in
this sample. Though the analysis of 120 holograms
is in progress, we confirmed that Eu occupies the
Ca site as expected.
The results obtained from BL10 indicate thathighly accurate local structure studies are possible
by neutron ARH at J-PARC. Because of the importance of light atoms in functional materials, the neutron ARH will impact strongly the materials science.
Since Japan is a leading country in this field, theneutron ARH experiments will be an important contribution of J-PARC to the world.

References[1]	K. Ohoyama, and K. Hayashi, Isotope News,
724, 14 (2014) in Japanese.
[2]	K. Hayashi, N. Happo, S. Hosokawa, W. Hu,
and T. Matsushita, J. Phys.: Condens. Matter,
24, 093201 (2012).
[3]	L. Cser, G. Krexner, and Gy. Török, Europhys.
Lett. 54, 747 (2001).
[4]	B. Sur, R. B. Rogge, R. P. Hammond, V. N. P.
Anghel, and J. Katsaras, Nature 414, 525 (2011).
[5]	K. Hayashi, K. Ohoyama, S. Orimo, Y. Nakamori,H. Takahashi, and K. Shibata, Jpn. J. Appl. Phys.
47, 2291 (2008).

K. Ohoyama1,2, K. Hayashi2, S. Hosokawa3, N. Happo4, M. Harada5, and Y. Inamura6
1
Advanced Institute for Materials Science, Tohoku Univ.; 2Institute for Materials Research, Tohoku Univ.; 3Dept. Phys., Kumamoto Univ.;
4
Hiroshima City Univ.; 5Neutron Source Section, Materials and Life Science Division, J-PARC Center; 6Neutron Science Section, Materials
and Life Science Division, J-PARC Center

4

Research and Development Highlights

Magnetic Frustration in 5d Iridium Spinel CuIr2S4
Investigated by Muon Spin Relaxation

2. µSR measurement
We employed DΩ-1 spectrometer at D1 experimental area, MLF, J-PARC and M15 beamline at
TRIUMF to measure zero-field / longitudinal-field(ZF/LF) µSR of (Cu1-xZnx)Ir2S4. The zero-field time
spectra are shown in Fig.1a. The development of
the exponential component at low temperatures indicates that a glassy magnetism develops in CuIr2S4.
The longitudinal response (Fig.1b), which could be
described by the theoretical curves for static magnetism, confirms the glassy magnetism. The magnetic
ground state changes when Zn ions are substituting Cu. Fig.1c and d indicate the zero-field muon
spin relaxation for Zn substituted samples. With avery small doping of ~ 1%, the magnetic response

0.10

CuIr2S4(x = 0.00)
ZF-µSR

0.05
0.00

LF =
40 mT
20 mT
10 mT
5 mT
2 mT
1 mT
ZF

(b)

0.20
0.15
0.10
2K
LF-µSR

0.05
0.00

Asymmetry

0.15

0

2

4

6

Time (µs)

8

(e)

0.20

200 K
100 K
60 K
40 K
2K

10

65 K
50 K
5K

0.15

Topical Results

(a)

0.20

0.10
(Cu1−xZnx)Ir2S4
x = 0.01
ZF-µSR

0.05
0.00

(f)

50 K
2K

0.20

Asymmetry

Asymmetry

0.25

Asymmetry

1. Introduction
Lately, 5d transition metal oxides are drawing
considerable interest, as they might exhibit an unconventional ground state due to the strong spinorbit (SO) coupling comparable with electron correlation. The strong SO coupling entangles the spinand orbital degrees of freedom, where the magnetic interaction of edge-shared Ir4+O6 octahedra ismodeled by the quantum compass model [1]. The
form of the exchange interaction depends on thespatial orientation of a given bond, leading to highly
anisotropic (Ising type) interaction between the Ir
ions.
In real materials, CuIr2S4 in its insulating phasewould serve as an ideal stage of the quantum compass model, as it partly comprises an edge-shared
Ir4+S6 network. We investigate the magnetic groundstate of (Cu1-xZnx)Ir2S4 using muon spin relaxation(µSR) [2]. The average charge state of CuIr2S4
yields Ir+3.5 and exhibits a disproportionation to Ir3+
(S = 0) and Ir4+ (Jeff = 1/2) below the metal to insulator transition of TM-I ~ 230 K [3]. The Zn2+ ions substituting Cu+ site introduces electrons onto the Ir site,
partially lifting the frustration of the Ir4+ network by
increasing the number of non-magnetic Ir3+ ions.

0.15
0.10

(Cu1−xZnx)Ir2S4
x = 0.1
ZF-µSR

0.05
0.00

0

2

4

6

Time (µs)

810Figure 1.	Muon spin relaxation spectra of (Cu1−xZnx)Ir2S4.
(a): in zero-field and (b) in magnetic field applied
parallel to the muon spin direction (longitudinal
fields). (c) and (d): Muon spin relaxation for doped
samples.

is diminished and both the amplitude and the rate of
the exponential relaxation are reduced.
3. Discussion and Conclusion
In Fig.2, the schematic arrangements of Ir3+ and4+
Ir of CuI2S4 are shown below the M-I transition.
Although Ir3+ has neither spin nor orbital degrees of
freedom, Ir4+ has them both alive: spin S = 1/2 andorbital L = 1. With the spin-orbit (SO) coupling within
the single Ir4+ ions, L + S = Jeff = 1/2 spin becomesthe good quantum number. The interaction between
the neighboring Ir4+ ions becomes strongly anisotropic and orientational-dependent from the orbital
part of Jeff = 1/2 spins. This situation is described byquantum compass model, in which many degrees
of freedom are frustrated [1]. Together with M-I transition, CuIr2S4 exhibits a crystal structural change tooctamer formation of Ir4+ network [3]. With the SO
interactions ignored, this octamer formation lifts thegeometrical frustration of S = 1/2 spins by tiling spin
singlets consistently on the shortened Ir-Ir bonds[3]. This “octamer singlet” formation of CuIr2S4 results to a non-magnetic singlet state, which is disproved by our µSR measurement.

Research and Development Highlights

5Topical Results

The spin glass ground state observed in µSR
measurement of CuIr2S4 suggests that some frustration is not perfectly lifted after the octamer formation. By substituting Ir4+ with non-magnetic Ir3+ asin (Cu1-xZnx)Ir2S4, the ground state becomes nonmagnetic, suggesting that the frustration is lifted by
the non-magnetic doping. There has been no microscopic model for the cause of the left-over frustration, but the SO interaction of Ir ions should play animportant role in the magnetism of CuIr2S4 spinels.

Figure 2.	Quantum compass model on the Ir4+ octamer of
CuIr2S4. Jeff = 1/2 spin which has an orbital component yields directional dependent interaction of
Ising type.

References[1]	G. Jackeli and G. Khaliullin, Phys. Rev. Lett.
102, 017205 (2009).
[2]	K. M. Kojima et al., Phys. Rev. Lett. 112, 087203,(2014).
[3]	P. G. Radaeli et al., Nature 416, 155, (2002).

K. M. Kojima1,2, R. Kadono1,2, M. Miyazaki1,2, M. Hiraishi1,2, I. Yamauchi1, A. Koda1,2, Y. Tsuchiya3, H. S. Suzuki3,
and H. Kitazawa3
1
Muon Science Section, Materials and Life Science Division, J-PARC center; 2Insitute of Materials Structure Science, KEK; 3Quantum Beam
Unit, National Institute for Materials Science, (NIMS)

6

Research and Development Highlights

SuperHRPD Finds Tiny Ru-O Bond Increments as Small as
0.0005 Å in Itinerant Ferromagnetic SrRuO3

2.	SrRuO3: Invar effect and Itinerant ferromagnetism
An+1RunO3n+1(A = Sr, Ca) is Ruddlesden-Popper
series, which shows various physical phenomena
with structural modification [2]. i. e. Sr2RuO4(n =1) is rare example of triplet superconductor while
Ca2RuO4 is Mott insulator. SrRuO3(n = ∞) is ferromagnetic while CaRuO3 is paramagnetic.
SrRuO3 and CaRuO3 are distorted ABO3
perovskite with same Pbnm space group (SG 62,

a-a-c+) from Ideal cubic Pm-3m (SG 221, a0a0a0).
Glazer categorizes Glazer tilting system to describe
distorted perovskite effectively by tilting rigid octahedron. Minus ‘-’, plus ‘+’, zero ‘0’ represent out-ofphase tilting, in-phase tilting and no tilting of neighboring octahedrons respectively.
SrRuO3 is a rare example of itinerant ferromagnetic among the 4d oxides. Even though spatiallyextended 4d orbitals, it has quite large magnetic
moment ~1.4 μB/Ru and high ferromagnetic transition temperature Tc = 165 K. It also shows zero thermal expansion, the so called Invar effect, and thechange of resistivity is below Tc. While bulk CaRuO3
doesn’t show any magnetic transition even though it
is near the verge of ferromagnetic instability. Tensilestress can induce ferromagnetic state in CaRuO3
film by lattice mismatch of the substrate [6]. The
Goodenough-Kanamori-Anderson (GKA) rule withorbital configuration explained successively the 3dlocalized magnetism. But the GKA rule couldn’t explain the itinerant ferromagnetism in SrRuO3.
The physical properties of Ru ruthenates arevery sensitive to tiny structural differences. Even
though the crystal structure and ferromagnetic
mechanism of SrRuO3 are strongly correlated witheach other, their detail relations are still unclear due
to limitation of the diffractometer resolution. The
SuperHRPD (BL08) beamline has been operatingin MLF, J-PARC. At present, the highest resolution it
approaches is Δd/d = 0.035%.
Thus, to understand the Invar effect and the ferromagnetic properties of SrRuO3 compared withparamagnetic CaRuO3, we carried out Time-of-flight
powder neutron diffraction with temperature scanfrom 10 K to 300 K at SuperHRPD in J-PARC [7].
We were able to measure the temperature dependence of the Ru-O bonds, which has not been detectable by the poor resolution diffractometer in previous studies.
RuO6 octahedron has already been distorted on
in-plane at room temperature. Ru-O bonds show

Research and Development Highlights

Topical Results

1. Introduction: 4d & 5d novel oxides
A strongly correlated electron system displays
numerous physical phenomena, i.e. multiferroics,
high Tc superconductor, quantum spin system andetc. with the coupling of lattice, spin, orbital andcharge degree of freedom.
Among the current active research fields, thetarget of major efforts is the attempt to find novel
magnetic phenomena in 4d and 5d oxides. In general, these 4d and 5d orbitals have more extended
orbitals than the 3d orbitals [1]. Then they have lessCoulomb interaction U and exchange interaction J.
Also, their large spin-orbit coupling is proportional toatomic number ~Z4.
For the 5d Ir oxides, Sr2IrO4 shows unexpectedMott insulator since large spin-orbit coupling opens
band gap with total spin Jeff = 1/2 [2]. A2IrO3(A = Li,Na) have been described in the Kitaev-Heisenberg
model [3]. Researchers are trying to find real Kitaev
spin liquid system with strong spin-orbit coupling
limit in the Kitaev-Heisenberg model. For 4d Ruoxides, Ru t2g orbital ordering reduces dimensionality from three dimensional networks to one dimensional Haldain chains effectively in Tl2Ru2O7 [4].
Li2RuO3 is considered by spin liquid system inducedby spin dimerization, which show the abrupt changeof magnetic susceptibility and structure simultaneously [5]. These 4d and 5d novel magnetic materials stimulate the development of both theory andexperiments.

7

Topical Results

temperature dependence, which means that the octahedron is not rigid and deviates from the Glazer
tilting assumption. In the Pbnm space group, latticea is always smaller than lattice b under a rigid octahedron. We took into account the lattice constants
with in-plane octahedron deformation that captures
the anomaly of lattice inequality a > b. In addition,
the octahedron becomes more symmetric at low
temperature. This experimental result is quite different from LDA+U calculation which predicts that the
Ru t2g orbital ordering favors ferromagnetic groundstates [8]. SuperHRPD detected tiny mean bond
<Ru-O> increment of about 0.0005 Å below ferromagnetic transition. Ru magnetic moments and<Ru-O> bond increments follow mean field curve ofmagnetization altogether. Finally, we compared the<Ru-O> bonds and the Ru 4d-O 2p band width W
obtained from empirical formula with paramagnetic
CaRuO3 and the reference of Colossal MagnetoResistance (CMR) La0.75Ca0.25MnO3 [9]. The <RuO> bond of paramagnetic CaRuO3 follows usual
thermal expansion while itinerant ferromagnetic
SrRuO3 shows increments of +0.0005 Å and CMR
La0.75Ca0.25MnO3 shows decrements of -0.005 Å
below Tc. The structural variation of SrRuO3 is oneorder smaller than CMR La0.75Ca0.25MnO3. The
bandwidth of CaRuO3 keeps constant in the wholetemperature range. But SrRuO3 decreases its bandwidth while La0.75Ca0.25MnO3 increases it. The increment <Ru-O> bonds and the localized bandwidth
contribute to the Invar effect and possibly the ferromagnetism mechanism respectively in SrRuO3.
Most high resolution neutron diffractometers canfind new relationships in strongly correlated electron systems, such as their structure and physicalproperties, which have not been accessible before
due to the limitation of resolution.

Figure 1.	Glazer tilting description (Pbnm, a-a-c+). Mean
<Ru-O> and <Mn-O> bond of itinerant ferromagnetic SrRuO3, paramagnetic CaRuO3 and CMR
La0.75Ca0.25MnO3.

References[1]	Eva Pavarini et al., Correlated Electrons: From
Models to Materials Modeling and Simulation
Vol. 2 Forschungszentrum Jülich (2012).
[2]	B. J. Kim et al., Phys. Rev. Lett. 101 (2008)
076402.
[3]	Yogesh Singh et al., Phys. Rev. Lett. 108,
127203 (2012).
[4]	Seongsu Lee et al., Nat. Mater. 5 (2006) 471.
[5]	G. Jackeli and D. I. Khomskii, Phys. Rev. Lett.
100 (2008) 147203.
[6]	S. Tripathi. et al., Sci. Rep. 4 (2014) 3877.
[7]	Sanghyun Lee et al., J. Phys.: Condens. Matter
25 (2013) 465601.
[8]	H-T. Jeng et al., Phys. Rev. Lett. 97 (2006)
067002.
[9]	P. G. Radaelli et al., Phys. Rev. B 56 (1997)
8265.

S. Lee1,2, S. Torii1,2, T. Kamiyama1,2, and J.-G. Park3
1
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Insitute of Materials Structure Science, KEK; 3Center for
Correlated Electron Systems, Institute for Basic Science (IBS), Seoul 151,747, Korea

8

Research and Development Highlights

Visualization of Magnetic Field Distribution by Polarized Pulsed
Neutron Imaging Inside the Power Magnetic Instrumentsb) Magnetization // Z

50

50

40

40

Y axis (ch)Y axis (ch)a) Magnetization // X

3020c) Hysteresis loop

30
20

10
0

Topical Results

Figures 1a) and 1b) show the magnetic moment
distribution of the annealed amorphous foil of 25 µm
in thickness measured by the polarized pulsed neutron imaging experiments. Because the sample wassettled in a magnetic shield box, the results shouldreflect its residual magnetization state. Fig. 1a)shows the distribution of magnetization components
along the horizontal direction (parallel to the X axis),
where the red color means positive sign and theblue indicates negative one. Also, the corresponding magnetization vectors in the XY plane, whichlies in the foil plane, are indicated by arrows. All thevectors are almost oriented in +Y direction (upwardin this figure), but in the red area they incline to theleft as they do to the right in the blue area. These
areas can be recognized as “magnetic domains”,
and their shape change by applying magnetic field
is connected directly to the magnetization process.
This is the first result showing that the magnetic domains of amorphous foil can be observed throughthe transmission technique.
The hysteresis loops of this sample, shown in
Fig. 1c), suggest that the easy axis is oriented to
the L direction, which is the same as Y direction.
Therefore, our results showing that the averaged
magnetization vector under zero magnetic field isdirected to the Y direction, is consistent with the result of the hysteresis loops

The loss reduction of power magnetic instruments such as motors and transformers is an urgent issue in preventing global warming because
the loss produces heat increase. In order to reduce
the loss, we have to design these equipment in suitable, however, we have little methods to inspect
the design directly. In power magnetic instruments
both the performances of magnetic materials andthe magnetic field designs are important. The polarized pulsed neutron imaging developed in MLF [1]should be able to visualize both the distribution of
the material magnetization and the magnetic field,
so it is a promising method for magnetization analysis. An expected application is the motor analysis,by measurement of both the motor gap magnetic
field and the motor core magnetization. The polarized pulsed neutron imaging in MLF is carried out at
beam line BL10.
Among possible magnetic materials to be used
for the motor core, amorphous films are expected toreduce the core loss significantly because of theirsmall coercive forces. But they are also extremely
sensitive to the stress produced in motor fabrication, which degrades their performance. The degradation could be reduced if the magnetic moments
motion inside the motor core is visualized, so theobservation through the core is important for the
motor design.

Magnetic vectors in XYplane
0

10

20

30

40

X axis (ch)

50

10
0

Magnetic vectors in XZ plane
0

10

20

30

40

50

X axis (ch)Figure 1. Magnetic domain observation by polarized pulsed neutron imaging.

Research and Development Highlights

9Topical Results

Figure 1. Motor observation by polarized pulsed neutron imaging.

On the other hand, Fig. 1b) shows the distribution of the magnetization component parallel tothe beam propagation direction (Z axis), which isnormal to the foil surface, and the arrows in thisfigure indicate magnetic vectors in the YZ plane.
Similar magnetic domain structure as in Fig. 1a)
was observed. This indicates the presence of perpendicular magnetization due to the perpendicularmagnetic anisotropy. While this magnetization component is known as the reason for the degradationof magnetic performance, the presence of such amagnetic component inside the foil was confirmed
experimentally for the first time.
Figure 2 shows the result of the motor gap observation. Fig. 2a) shows the model motor fabricated as frameless type so that the motor gap is open
and observable by the eye. The stator and the rotor
were held with an aluminum frame and an axe, so
the holder caused neither neutron depolarization
nor any distortion in the magnetic field distribution.
On the rotor surface 4 crescent type magnets arestuck and the stator consists of 15 yoke teeth withcoils wound by distributed type. Fig. 2b) shows
the gap field in absolute value calculated without

the coil current. At the center of the gap the maximum magnetic field intensity was 5 kOe. Figure 2c)shows the neutron transmission image of the motor
sample. The opaque area at the center of this image corresponds to the rotor, and the surrounded
ring-shaped bright area does the motor gap. The
polarization image of the motor is shown in Fig. 2d).
The neutron spin was along the Y axis. At both sidesof the rotor, the neutron polarization kept its initialvalue, but it turned to zero in the other area. This result indicates that the neutron spin direction and themagnetic field direction were parallel to each otherat both sides of the rotor that corresponds to thecalculated field direction. Thus, we can analyze thedirection of the magnetic field in the motor gap bymeans of the polarized neutron imaging technique.
From these results the polarized pulsed neutron
imaging is found to be a powerful tool for magnetic
analysis of the motor magnetization.
Reference[1]	T.Shinohara et al., Nucl. Instrum. Meth., A 651,
121 (2011).

T. Imagawa1, T. Hirano1, K. Souma2, T. Shinohara3, and H. Hayasida4
1
Hitachi, Ltd.; 2Hitachi Industrial Equipment Systems Co., Ltd.; 3Neutron Science Section, Materials and Life Science Division, J-PARC
Center; 4Neutron R&D Division, CROSS-Tokai

10

Research and Development Highlights

Detection of High Elastic Strain in Fe3Pt Using TAKUMI

Lattice parameter (nm)

0.38
0.37
0.36
0

50

100
150
200
Temperature (K)

250

300

direction because the largest elastic strain is expected in this direction when softening in C’ occurs.
2. Experiments
A single crystal of Fe3Pt was grown by the floatingzone method, and a specimen with dimensions of
9.8 mm × 2.6 mm × 2.5 mm was cut out. The specimen was heat-treated at 1373 K for 24 h and thenat 923 K for 100 h to obtain the ordered L12-type
structure with S = 0.75. The specimen of Fe3Pt wascompressed in the [001] direction at 93 K, which isslightly above the transformation temperature. The
002 reflection was detected by the + 90° detector,and 220 reflection was detected by the - 90° detector as schematically shown in Fig. 2.

Crystallography

1. Introduction
In most metals and alloys, the elastic limit obtained by experiments is less than 1%, although thefirst principle calculations suggest it may exceed
10%. It is well known that the movement or creationof dislocations prevent high elastic strain.
Exceptionally high elastic strain is known to appear in alloys with high elastic anisotropy (C44/C’).
For example, a large elastic strain of more than
1% was reported in Cu-Al-Ni and Ni-Mn-Ga shapememory alloys. Considering the high elastic strain inthese alloys, we may expect that a very high elasticstrain can be obtained when the elastic anisotropy
becomes very large.
A representative alloy, in which we can expect
very high elastic anisotropy, is a partly ordered
Fe3Pt with degree of order 0.75. This alloy exhibits
second order like martensitic transformation from a
cubic (L12-type) structure to a tetragonal (L60-type)structure near 90 K in the cooling process. The lattice parameters change continuously as shown in
Fig. 1. Because of the softening in C’ associatedwith the transformation, the anisotropy (C44/C’) is
expected to become extremely high in the vicinity ofthe transformation temperature.
In the present study, we examined the elastic deformation of Fe3Pt under the compressive stress applied in the [001] direction by using BL19 (TAKUMI)
at J-PARC. We selected [001] as the compressive

Figure 2. Experimental setup at BL19 TAKUMI [2].

3. Lattice Strain under stress
From the peak position of 002 and 220 reflections, we obtained the lattice parameters c and aunder compressive stresses as shown in Fig. 3. We
notice in Fig. 3 that c and a both change continuously and almost linearly. The change in c and a causedby the stress application exceeds the one producedby the temperature change from 90 K to 10 K.
Figure 4 shows the lattice strain (elastic strain)calculated by using the following equation:

Figure 1.	Temperature dependence of lattice parameters of
Fe3Pt [1].

Research and Development Highlights

11

Crystallography

Figure 3.	Stress dependence of lattice parameters at 93 K [2].

εL =c − c0
× 100
c0

(1)


It is clear that the lattice strain exceeds 6%. The
strain agrees with that obtained by attaching a strain
gage [3]. The Young’s modulus obtained by the slopeof Fig 4 is 4.7 GPa, being one order in magnitude
smaller than that of conventional metals and alloys.
4. Summary
We confirmed by using TAKUMI that an Fe3Pt
with degree of order 0.75 exhibits a very large

Figure 4. Stress dependence of lattice strain.

elastic strain of more than 6% when compressed inthe [001] direction near 90 K.
References[1]	T. Fukuda, T. Sakamoto, T. Kakeshita, T. Takeuchi
and K. Kishio, Mater. Trans. 45 (2004) 188.
[2]	T. Yamaguchi, T. Fukuda, T. Kakeshita, S. Harjo
and T. Nakamoto, Appl. Phys. Lett. 104 (2014)
231908.
[3]	T. Fukuda and T. Kakeshita, Scripta Mater. 69(2013) 89.

T. Fukuda1, T. Yamaguchi1, T. Kakeshita1, S. Harjo2, and T. Nakamoto3
1
Department of Materials Science and Engineering, Graduate School of Engineering, Osaka University; 2Neutron Science Section, Materials
and Life Science Division, J-PARC center; 3High Energy Accelerator Research Organization, KEK

12

Research and Development Highlights

1. Introduction
Transformation Induced Plasticity (TRIP) is
one of important effects in the steel strengthening
mechanism to improve strength and ductility, andto achieve an excellent high-speed deformation behavior. As shown in Figure 1, TRIP steels show highstrength with relatively large elongation. Moreover,
TRIP steels also show excellent shock absorption
in case of collision, and therefore are applied in the
body of cars.
The TRIP effect, as shown in Figure 2, occurs insteel containing a metastable phase (A phase), in
which the A phase transforms into a different phase(M phase) during plastic deformation. Because the Mphase steel is known to have high strength, the highstrength of TRIP steels is predicted to be due to thetransformation from the A to the M phases. However,there were almost no quantitative researches on thisbehavior to bring the TRIP effect, which showed the
direct contribution of the M phase to the strength. We
were challenged to understand this behavior using
the neutron diffraction (ND), because this techniqueis the most appropriate tool to get microstructural
information as bulk average. These kinds of studies
have been conducted previously with un-satisfied results, because the separation of diffraction peaks ofthe matrix F and M phases could not be obtained dueto the limited resolution of the instrument used [1].

Figure 1.	
Strength and elongation properties of various
steels.

Crystallography

Strengthening Mechanism of Advanced Steelwith Deformation Induced Phase Transformation

Figure 2. Illustration of TRIP effect.

2. Experiments
In situ neutron diffraction measurements duringloading of a TRIP steel specimen with A phase volume fraction of about 11% was conducted at room
temperature using TAKUMI which has the best resolution in Δd/d of about 0.17% [2]. Thanks to the neutron flux and the flexible data acquisition/reduction,measurements during plastic deformation region(where TRIP effect occurred) were challenged to be
conducted in a continuous manner. Conventionallythe measurements within the plastic region havebeen conducted by holding strain or displacement,
which might give low accuracy due to the occurrence of stress relaxation during the holding. The M
phase amount might also change during the holding.
Figure 3 shows that the (211) diffraction peaksof the matrix and M phase at the plastic deformation
region can be separated, because the stress relaxation was suppressed and therefore the accuraciesof the peak positions were high.

Figure 3.	
Diffraction pattern of (211) peaks at a plastic
deformation.

Research and Development Highlights

13

Crystallography

3. Results and discussions
Peak positions of several (hkl) peaks of threephases were carefully determined by the peak separation procedure shown in Figure 3. Lattice strains
during loading were then evaluated by comparing
the peak positions obtained during loading to thoseobtained before deformation. It is clear from Figure 4
that, lattice strain sharing occurs among {hkl} family
grains (intergranular strains) and also among constituent phases. The intergranular strains increase
with increasing the applied strain. The average lattice strains of the A phase seem higher than the matrix, showing that the A phase (retained austenitewith high carbon content) behaved as the harderphase compared to the matrix. The most interesting
one is that the M phase lattice strains were possible
to be estimated, and they show the largest values,
proving that the M phase formed during transformation is the hardest phase.
It is necessary to confirm quantitatively the contribution of the M phase to the whole strength. The
stress contribution from each phase can be estimated by multiplying the stress for each phase witheach volume fraction for the same applied stress or
strain condition. As shown in Figure 5, even though
the stress contribution of the M phase is small at
the early stage of the plastic region, it increases tobecome superior to that of the A phase at a large
applied stress region due to the increase of the Mphase volume fraction. When the balanced stresses
were calculated from the stress contributions of thethree phases using the mixture law, as it is clearlyshown in Figure 5, the stress contribution of the Mphase plays an important role in the whole strength.

Figure 5.	Stress contributions of the three phases in TRIP
steel during deformation [3].

Figure 4.	Lattice strains of typical {hkl} oriented grains asfunctions of applied strain [3].

References[1]	O. Muransky, P. Sittner, J. Zrnik, E.C. Oliver,
Acta mater. 56 (2008) 3367.
[2]	S. Harjo, T. Ito, K. Aizawa, H. Arima, J. Abe, A.
Moriai, T. Iwahashi, T. Kamiyama, Mater. Sci.
Forum, 681 (2011) 443.
[3]	S. Harjo, N. Tsuchida, W. Gong, J. Abe, K.
Aizawa, Mater. Res. Soc. Symp. Proc. 1528
(2013).

S. Harjo1, N. Tsuchida2, W. Gong1, J. Abe1, and K. Aizawa1
1
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Graduate School of Engineering, University of Hyogo

14

Research and Development Highlights

Diffraction Study of High Neutron Absorbing Material EuGa4
on SENJU

2. Experiments and results
A single crystal EuGa4 with size 5 × 3 × 1.5 mm3

was used for the experiment. Note that Eu in thepresent sample is not enriched by 153Eu isotope but
the natural one. The diffraction patterns were measured at 20.6 K (above TN) and 4.2 K (below TN).
The wavelength range of an incident neutron was
0.4 Å ~ 4.4 Å at first-frame. Significant numbersof diffraction spots were clearly observed in spiteof the high neutron absorption of Eu as shown in
Figure 1. The obtained lattice parameters of a = b= 4.376(2) Å and c = 10.648(4) Å at 20.6 K agreed
well with the values determined by X-ray diffraction.
Diffraction intensities on (h0l)* reciprocal latticeplane at 20.6 K and 4.2 K were plotted in Figure 2.
The magnetic reflections were clearly observed at
the positions of h + k + l ≠ 2n at 4.2 K. The positionsof these reflections indicated an antiferromagnetic
ordered structure with propagation vector q = 0.

Crystallography

1. Introduction
Single crystal neutron diffraction provides fundamental but essential information about the structuraland magnetic properties of materials. However, in
neutron diffraction experiments it is problematic touse compounds containing rare earth elements like
Sm, Eu, Gd, and Dy, because they are known ashigh neutron absorbers. Using a pulsed neutron,
which includes a short wavelength, reduces the effect of neutron absorption by the sample, and allows efficient data collection. The time-of-flight neutron diffractometer SENJU at BL18 should becomea powerful tool to study high neutron absorbing
compounds.
EuGa4 has a BaAl4-type structure with I4/mmm
symmetry and is considered a parent compoundof the so-called 122 compounds that are rich inphysical properties, including superconductivity andvalence fluctuation. The bulk properties of EuGa4
indicate an antiferromagnetic order at 16 K [1].
However, the magnetic structure of the compoundis still unknown. The neutron diffraction experiment[2] was carried out to determine the effectiveness of
SENJU in studying the high absorbing compounds
and obtaining the structural information of an antiferromagnetic ordered EuGa4.

3. Summary
Nuclear and magnetic reflections of EuGa4
were successfully observed. Both crystal and magnetic structural information of Eu-based compound
can be obtained on SENJU taking advantage of awide wavelength range and large area detectors.
Extensive studies on the magnetic properties ofrare-earth based compounds, containing high neutron absorbing elements, will be conducted using
the TOF neutron diffraction.

Beam+22.5°+157.
2θ

-115.5°-67.5rFigure 1. Neutron diffraction pattern of EuGa4 on the detectors of SENJU at 20.6 K.

Research and Development Highlights

15

Crystallography

Figure 2. Neutron diffraction intensities on (h0l)* reciprocal lattice plane.

References[1]	A. Nakamura, Y. Hiranaka, M. Hedo, T. Nakama,
Y. Miura, H. Tsutsumi, A. Mori, K. Ishida, K.
Mitamura, Y. Hirose, K. Sugiyama, F. Honda, R.
Settai, T. Takeuchi, M. Hagiwara, T. D. Matsuda,
E. Yamamoto, Y. Haga, K. Matsubayashi, Y.
Uwatoko, H. Harima and Y. Ōnuki: J. Phys. Soc.

Jpn., 82 (2013) 104703.
[2]	T. Kawasaki, K. Kaneko, N. Aso, A. Nakamura,
M. Hedo, T. Nakama, Y. Ōnuki, T. Ohhara, R.
Kiyanagi, K. Oikawa, I. Tamura, A. Nakao, K.
Munakata, T. Hanashima: JPS Conf. Proc., 1(2014) 014009.

T. Kawasaki1, K. Kaneko1,2, N. Aso3, A. Nakamura4, M. Hedo3, T. Nakama3, Y. Ōnuki3, T. Ohhara1, R. Kiyanagi1, K. Oikawa1,
I. Tamura1,5, A. Nakao6, K. Munakata6, and T. Hanashima6
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Quantum Beam Science Center, JAEA; 3Graduate School ofEngineering and Science, University of the Ryukyus; 4Faculty of Science, University of the Ryukyus; 5Department of Research Reactor andTandem Accelerator, JAEA; 6Neutron R&D Division, CROSS-Tokai

16

Research and Development Highlights

Crystal Structures and Hydrogen Bonding in High-pressureand High-temperature Phases of Ca(OD)2

2. Experimental
An initial sample of powder Ca(OD)2 wassynthesized from a mixture of CaO powder and excess D2O in an autoclave at ­220°C for 1 week. HighPT experiments were conducted using the multianvil apparatus with six independently acting 500t
rams (6-axis press called “ATSUHIME”) at the newhigh-PT beamline “PLANET”. The neutron diffraction patterns were measured at 8.5 GPa under decreasing temperature from ­400°C, ­200°C, to room
temperature. High-P experiments at room temperature were performed using a new anvil assembly[8], which was installed into a Paris-Edinburgh (PE) press. The diffraction pattern of the high-P phase
was obtained at 11 GPa. The lattice parameters andatomic positions were refined by Rietveld analyticalmethod using GSAS software. The initial structure
models were taken from previous studies [4-6].
Complementary data on the hydrogen bonds in
Ca(OD)2 were obtained via Raman spectroscopy in
the region of the OH stretching vibration mode fromseparate experiments using a diamond anvil cell.

Crystallography

1. Introduction
Calcium hydroxide (portlandite) belongs to brucite-type layered hydroxides with a CdI2 structure,
which has hydrogen bonds within the interlayer of
MO6 octahedral sheets. Pressure-induced changes
in hydrogen bonding are important not only in materials science and crystallography, but also in geoscience, because these layered hydroxides are considered to be a model structure of hydrous minerals
that transport water into the deep Earth.
Among the other isostructual hydroxides, portlandite has the largest Ca cation, which mightcause unique pressure-induced phase transitions.
Previous studies reported that portlandite undergoes a phase transition to a high-pressure (high-P)
phase at 6–8 GPa and room temperature [1-3], andtransforms into another high-pressure and hightemperature (high-PT) phase at > 6 GPa, > ­200°C[4, 5]. The crystal structures of both phases havebeen determined by X-ray and/or neutron diffraction
measurements [5, 6]. However, no in-situ neutron
observation has been conducted previously undersuch high-PT conditions that the high-P and high-PT
phases are stable. This is presumably due to technical difficulties of the high-P neutron diffraction andthe characteristics of the sample; the single high-P
phase can be obtained only under hydrostatic conditions above 10 GPa, still showing very weak signal. Furthermore, both high-P and high-PT phases
are normally unquenchable at ambient condition.
In the present study, therefore, in-situ neutron
diffraction measurements under high-P conditions
were performed in order to clarify the unknownhydrogen positions in the various polymorphs. To
overcome the previous difficulties described above,
we used two different high-P apparatuses with recently developed techniques and improved accessible PT conditions [7].

3. Results and discussion
Fig. 1 shows representative diffraction patternsof (a) the high-P phase measured at 11 GPa, room
temperature using the P-E press, and (b) the highPT phase measured at 8.5 GPa and ­400°C using the
6-axis press. The refined crystal structures of bothphases are shown in Fig. 2. The hydrogen positions
for the high-P phase were first clarified. The hydrogen bonds in the high-P phase orientate randomly
between the CaO polyhedral layers under high pressure. According to the obtained O(–D)...O distances
and angles, the hydrogen bonds are bent and theirstrength is relatively weak, but slightly getting stronger with increasing pressure. The geometry of thehydrogen bond was quite consistent with the resultsfrom Raman spectroscopy. The structure of the highPT phase was concordant with that observed previously in Ref. [5] for a recovered sample. Based on
the obtained structures of the Ca(OD)2 polymorphs,
the phase transition mechanism involves the sliding

Research and Development Highlights

17

Intensity (a.u.)

(a)

(a)

10

15

20

25

30

(b)

35
c

(b)
Crystallography

Intensity (a.u.)

a

c

5

10

15

20

25

30

b

TOF (ms)

Figure 1.	Neutron diffraction patterns of (a) high-P phaseand (b) high-PT phase. “+” denotes the observed
data points; the solid line denotes the calculated
profile. Tick marks below the pattern show thepositions of diffraction peaks calculated for (a) Ni(green), WC (black), and high-P phase (red), and(b) high-PT phase (red). The difference between
the observed and the calculated profiles is shownby a blue line at the bottom of each plot.

Figure 2.	Crystal structures of Ca(OD)2 (a) high-P phaseand (b) high-PT phase. The biggest blue atom denotes Ca; the middle red atom oxygen, and thesmallest white atom deuterium. For comparison,both structures are shown along corresponding
directions (details in [6, 7]).

of the CaO polyhedral layers, position modulationsof the Ca atoms, and recombination of the Ca–O
bonds as shown in Fig. 2. The high-P phase seems
metastable and transforms into the high-PT phase athigh temperature with accompanying further structural relaxation and reorientation of the hydrogenbonds to form more stable hydrogen bonds.

[3]	Iizuka et al., Phys. Chem. Minerals, 38, 777–785 (2011).
[4]	Kunz et al., High Press. Res., 14, 311–319(1996).
[5]	Leinenweber et al., J. Solid State Chem., 132,
267–273 (1997).
[6]	Iizuka et al., American Mineralogist, 98, 1421–
1428 (2013).
[7]	Iizuka et al., J. Solid State Chem., 218, 95–102(2014).
[8]	Iizuka et al., High Press. Res., 32, 430–441(2012).

References[1]	Ekbundit et al., J. Solid State Chem., 126, 300–
307 (1996).
[2]	Catalli et al., Geophys. Res. Lett., 35, L05312(2008).

R. Iizuka1,2, K. Komatsu3, H. Kagi3, T. Nagai4, A. Sano-Furukawa5, T. Hattori5, H. Gotou6, and T. Yagi3
1
Geodynamics Research Center, Ehime University; 2Bayerisches Geoinstitut, Universität Bayreuth, Germany; 3Geochemical Research Center,
Graduate School of Science, The University of Tokyo; 4Division of Earth and Planetary Sciences, Graduate School of Sciences, Hokkaido
University; 5Neutron Science Section, Materials and Life Science Division, J-PARC center; 6Institute for Solid State Physics, The Universityof Tokyo

18

Research and Development Highlights

Neutron Crystal Structure Analysis of Human
α-Thrombin-Inhibitor Complex using iBIX

Figure 1. α-Thrombin-bivalirudin complex.

3D structure of α-thrombin-bivalirudin complex after
the hydrolysis determined by X-ray crystallography.
Under the crystallization condition, two products remain to bind to the α-thrombin molecule due to thehigh concentrations. From enzymatic viewpoint, thecomplex is regarded as an Enzyme-Product (EP)complex. I have tried to determine the protonation
stats of the complex to understand the enzymaticmechanism of α-thrombin using neutron protein crystallography [1]. Since hydrolysis of serine proteaseinvolved migration of hydrogen atoms or hydrogenbond formations among protein, substrate and watermolecules, neutron crystallography is an adequate
tool to study the enzymatic reaction mechanism.
The neutron crystallography of α-thrombin-bivaliudin
complex is expected to provide information on theformation of the EP complex of serine proteases.

Crystallography

1. Introduction
α-Thrombin is a serine protease which plays acentral role in coagulation. It converts fibrinogen to
fibrin monomer, which forms fibrin fiber to become amain component of the blood clot. Direct α-thrombin
inhibitors (DTI) can be promising anticoagulant
agents because they work only on α-thrombin, unlike warfarin or heparins, which affect the functionsof many blot clot proteins. Bivalirudin is a DTI approved by FDA in US. It is a synthetic peptide whose
amino acid sequence is dFPR-P-GGGG-D53GDFEEIPEEYL64. It has two components connected with apoly glycine linker (GGGG). The N-terminal part, dFPRP, binds to and blocks the active site α-thrombin.
Here, dF stands for D-phenylalanine. The C-terminal
part following the linker is a part of hirudin, natural anticoagulant peptide from saliva of Hirudo medicinalis,the European medicinal leech. It binds to Exosite Iof α-thrombin and blocks binding of fibrinogen molecules. For that reason, bivalirudin is a divalent
anticoagulant, which has a small binding constant.
Bivalirudin is hydrolyzed by α-thrombin to dFPRCOOH and NH3-P-GGGG-D53GDFEEIPEEYL64.
Since those two components have large binding
constants for α-thrombin, the half-life of bivalirudin
is around 25 minutes in patients. Figure 1 shows the

2. Diffraction experiment
The crystal of α-thrombin-bivalirudin was grownby a sitting drop vapor diffusion method with fourtimes macro-seeding procedures. The sample size
was 3.5 mm3. The crystal was soaked in an artificial
mother liquor containing deuterium oxide to replace
H atoms with D atoms in the crystal, which helps toreduce the background due to incoherent scatteringof the H atoms. The sample was sealed in a quartz
capillary with small amount of the soaking solution.
The sample was mounted on MLF BL03 iBIX.
The beam power was 300 kW. The 25 Hz neutron
pulse beam was irradiated for around 8 hours foreach setting. The diffraction experiment was carried out at room temperature. To collect a data set
enough for the structure analysis, diffraction patterns for 24 settings of crystal orientations were collected with 30 wavelength-shift fiber type scintillation counters developed for iBIX. The data reduction
was carried out by using the program STARGazer
v.1.0.0-rc3. The event data were transformed to thehistogram data. Figure 2 shows a diffraction patterndetected by detector No. 10 (2θ = 51° at the detector

Research and Development Highlights

19

Table 1. Crystallgoraphic data.

X-ray

Space group, Za, b, c / Åβ/°Resolution / ÅRmergeRwork
Rfree

Neutron
C2, 4
71.04, 72.02, 72.36
100.5
36-1.6
20.4-2.0
0.033
0.119
0.165
0.172
0.180
0.230

Crystallography

Figure 2. A TOF Laue pattern.

center). The diffraction spots were indexed and theintensities were integrated to obtain the hklFo data.
After the neutron diffraction experiment, X-ray
diffraction experiments were carried out at Photon
Factory AR-NW-12 (KEK) using the same crystalline sample.
3. Structure Refinement
The X-ray/neutron joint refinement was carriedout using neutron and X-ray diffraction data sets,
dealing with the program PHENIX suite version
1.8.3. Molecular modeling was done by the program
Coot version 0.6. The crystallographic data, statistics for data collection and refinements extracted areshown in Table 1. The statistics indicates that qualityof the neutron diffraction data obtained by iBIX is decent and the refinement was carried out successfully.
The figure shows the 2mFo-DFc neutron scattering
length density map and the OMIT map for deuterium
atoms near the active site (drawn in cyan and magenta). Both maps show clear protonation of His57.

T. YamadaFrontier Research Center for Applied Atomic Sciences, Ibaraki University

20

Research and Development Highlights

Figure 3. Neutron 2Fo-Fc and OMIT maps.

His57 forms a hydrogen bond to Arg3 of the product,
not to Ser195. Hydroxyl group of Ser195 orients toVal213_O, although the length of O…D is little longat 2.5 Å. The freedom of the hydroxyl group might
be a key to ease the dissociation of the product fromα-thrombin to complete the hydrolysis reaction.
References[1]	T. Yamada et al., Biochim. Biophys. Acta, 1834
(2013) 1532.

Neutron Diffraction Study for Reaction Mechanismof RNase A by using iBIX

2. Neutron difftaction measurement
Neutron diffraction data set of bovine pancreatic
RNase A were collected by IBARAKI biological crystal diffractometer iBIX in J-PARC [4,5]. The crystal
of RNase A grew to 6.0 mm3 (2.5 × 2.4 × 1 mm) in
two weeks. The crystal was soaked in deuterated
solution for 10 days to reduce the background scattering from H atoms, which have a large incoherent
neutron scattering length.
The full data set for neutron structure analysis could
be obtained in 7 days at 300 kW operation of accelerator power at J-PARC. The exposure time was 4 hour
per setting. The total number of settings was 40. The
crystal data and measurement conditions are shownin Table 1. One of the typical TOF diffraction patterns
is shown in Fig. 1. The very sharp Bragg spots indicate that the quality of the crystal sample is sufficientto perform the neutron diffraction experiment.

Table 1. Crystal data and measurement conditions.

TemperatureSpace group
Unit-cell


a
b
c
β

Crystal size
Accelerator power
Range of wavelength
Exposure time
Total No. of settings
Total measurement time

(K)

(Å)
(Å)
(Å)
(°)
 (mm3)
 (kW)(Å)
 (hours) (days)

293
P21
30.4
38.6
53.4
105.8
6.0
280
1.6 ~ 4.6
4.0
40
7

Crystallography

1. Introduction
Bovine pancreatic ribonuclease A (RNase A) is aendoribonuclease that claves and hydrolyzes singlestranded RNA exclusively at pyrimidine nucleosidepositions in two distinct steps. The mechanism of thecleavage reaction catalyzed by RNase A involves
two key histidine residues, His12 and His119. It is
important to know the protonation states of themin order to understand the hydrolysis mechanismof RNase A. Neutron protein crystallography is a
powerful technique for problem solving. In previous
reports, the protonation states of His12 and His119
for RNase A complexed with phosphate ion, uridine
vanadate and phosphate free one have been investigated by neutron diffraction analysis [1-3].
In this study, neutron diffraction analysis of phosphate free RNase A has been carried out with highresolution and completeness data set collected byusing iBIX in order to clarify the protonation statesof two histidine residues in active site, and to elucidate the detailed mechanism of the cleavage reaction catalyzed by RNase A.

Figure 1.	TOF diffraction pattern of RNase A obtained by using
iBIX.

3. Structure analysis
The data reduction was carried out with the program STARGazer [4] developed for TOF diffraction
data measured by iBIX. The data reduction was
successfully completed and then the integrated intensities of the Bragg reflections could be obtained
for the structure refinement. A total of 20,513 uniquereflections were obtained with an overall Rsym of
13.5% from 67,740 observed reflections. The average of I/σ(I) and redundancy were 8.1 and 3.3
respectively. The crystal data, measurement conditions, and the statistic of the data reduction andrefinement are summarized in Table 2.

Research and Development Highlights

21

Table 2. The statistics of the data reduction and refinement.

No. of observed reflections
No. of unique reflections
Resolution(Å)
Completeness(%)
Average I/σ(I)Redundancy
(%)
Rsym
(%)
Rcryst(%)
Rfree

67,74020,513
1.4
86.7
8.1
3.3
13.5
19.4
22.0

Crystallography

The structure refinement was carried out using
the program phenix.refine including PHENIX-1.8[5]. The structure was determined by joint neutron
and X-ray structure refinement. 10% of reflections,randomly selected, were assigned as a test set forcross validation. The final values of Rcryst and Rfree

were 19.5% and 22.0%, respectively, for completeness of 86.7% to a resolution of 1.4 Å.
The structure with high reliability and good data
statistics could be obtained finally by comparing
with the already-reported one [3].
2|Fo|-|Fc| neutron scattering length map aroundthe active site including His 12 and His 119 is drawn
in Fig. 2. We also calculated the |Fo|-|Fc| neutron
scattering length density map after omitting Dδ1 andDε2 of His12 and His119 in order to confirm their
protonation states. These omit maps indicated that
His12 is completely singly protonated and Hi119
is doubly protonated. Their protonation states are
consistent with those in the first step of the putative
mechanism of catalysis by RNase A. We could also
observe a D atom of water molecule which is hydrogen bonded to Nε2 of His12.

Figure 2. TOF diffraction pattern of RNase A obtained by using iBIX.

References[1]	A. Wlodawer et al., Proc. Natl Acad. Sci. USA,80 (1983) 3628–3631.
[2]	A. Wlodawer, L. Sjölin, Biochemistry 22 (1983)
2720–2728.
[3]	D. Yagi et al., Acta Cryst. D65 (2009) 892–899.
[4]	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.
[5]	K. Kusaka, T. Hosoya, T. Yamada, K. Tomoyori,
T. Ohhara, M. Katagiri, K. Kurihara, I. Tanaka
and N. Niimura, J. Synchrotron Rad. 20 (2013)
994–99.
[6]	T. Ohhara et al., NIMA 600 (2009) 195–197.
[7]	P. Adams et al., Acta Cryst. D66 (2010)
213–221.

K. Kusaka1, T. Yamada1, K. Tomoyori2, T. Hosoya1, T. Ohhara3, I. Tanaka1, and N. Niimura1
Frontier Research Center for Applied Atomic Sciences, Ibaraki University, Tokai; 2Quantum Beam Science Center, JAEA; 3Neutron Science
Section, Materials and Life Science Division, J-PARC center

1

22

Research and Development Highlights

Local Structural Changes with Amorphization
on Thermal Decomposition Reaction of LiAl(ND2)4

3. Results and Discussion
Figure 1 shows the structure factor, S(Q), ofLiAl(ND2)4 (a) before and after heat treatment at (b)433 K and (c) 673 K [4]. The data were obtained
from the neutron scattering intensity, which wascollected using the 45° detector bank of the NOVA
spectrometer. During the heat treatment, the profile drastically changed from sharp diffraction peaks
to broad diffuse scattering features, indicating theamorphization of the sample.

0.40.3(a) RT

30
20
10

Liquid & Amorphous Science

2. Neutron Diffraction Measurements
The sample preparation of LiAl(NH2)4 is explained in a previous publication [3]. LiAl(ND2)4 wassimilarly prepared using LiD and ND3 instead of LiH
and NH3, respectively. For the purpose of structuralcharacterization of the decomposition products,
LiAl(ND2)4 samples heat-treated at 433 K and 673 K
were prepared using a heating rate of 5 K/min,
which was then immediately cooled to room temperature under helium gas flow. LiAl(ND2)4 (60 mg)
was examined before and after the decomposition
for an exposure time of 11 h by ex situ neutron diffraction on the neutron total scattering spectrometer
NOVA (BL21) connected to the 200 kW spallation
neutron source at J-PARC.

Lattice spacing, d/Å
1
4 3 2

10

0

Structure factor, S(Q)

1. Introduction
Lithium aluminum amide LiAl(NH2)4 is of interest
as a possible hydrogen storage material because
the composite material consisting of LiAl(NH2)4 and
LiH releases hydrogen gas by 6.1 mass% at temperatures below 400 K [1, 2]. A hydrogen desorption
mechanism of the composite has been proposed,
but it is still controversial because the decomposition mechanism of LiAl(NH2)4 is not well-understood. Our goal in the present report is to investigate the detailed structural properties before andafter the decomposition of LiAl(ND2)4 using neutron
total scattering and atomic pair distribution function(PDF) analysis.

(b) 433 K

30
20
10
0

(c) 673 K

30
20
10
0
4

5 6 7

1

2

3

4

5 6 7

10
-1
Momentum transfer, Q/Å

2

3

Figure 1.	Structure factors, S(Q), for the neutron scattering profiles of LiAl(ND2)4 (a) before and after heat
treatment at (b) 433 K and (c) 673 K [4].

Figure 2 shows the atomic pair distribution function, G(r), obtained by the Fourier transformation of
S(Q) for LiAl(ND2)4 before and after the heat treatment [4]. We assumed that LiAl(ND2)4 decomposes
to Li3AlN2 and AlN, shown as follows:(1 − x)LiAl(ND2)4→ (1/3)xLi3AlN2 + (2/3)xAlN + (8/3)xND3(1)
The PDF refinements of the G(r) profiles were performed in the region of 0.5 ≤ r ≤ 5.0 Å, which includes more than 500 bonding pairs (383 LiAl(ND2)4,113 Li3AlN2 and 64 AlN). Half and almost all of the

Research and Development Highlights

23

LiAl(ND2)4 decomposed at 433 K and 673 K, respectively. Therefore, we confirm that LiAl(ND2)4
decomposes to amorphous mixed phase including
Li3AlN2 and AlN. This preliminary report on our local
structural analysis, which includes the amorphization reaction, provides fundamental information not
only for the decomposition process of LiAl(NH2)4 but
also for the further study of possible hydrogen storage materials.

4(a) RT
x=0
Rwp 7.8%

2

Liquid & Amorphous Science

Acknowledgments
The authors would like to thank Mr. H. Oki and
Mr. T. Iwase for their helpful assistance in the neutron scattering experiments. The work presented
here is partially supported by the New Energy andIndustrial Technology Development Organization(NEDO) under “Advanced Fundamental Research
Project on Hydrogen Storage Materials’’ and“Feasibility Study on Advanced Hydrogen Storage
Materials for Automotive Applications (2012)”, JSPS
KAKENHI Grant Numbers 23686101, 24241034,
and the Neutron Scattering Program Advisory
Committee of IMSS, KEK (Proposal No. 2009S06).

Atomic pair distribution function, G(r)/Å

-2

0
-2
-4
(b) 433 K
x = 0.53
Rwp 11.7%

4
2
0
-2
-4
4

(c) 673 K
x = 0.92
Rwp 13.9%

2
0
-2
-4
1

2

3

4

4. Conclusions
We have attempted to elucidate the local structural changes that occur during the decomposition
process that accompanies the amorphization ofLiAl(ND2)4 using ex situ neutron total scattering measurements and PDF analysis. The structure factors ofLiAl(ND2)4 before the decomposition were characterized by isolated [ND2] units. Atomic pair distributionfunctions after the heat treatment at 433 K and 673 K
confirmed that LiAl(ND2)4 decomposed to amorphousmixed phases containing Li3AlN2 and AlN.

5

Distance, r/Å
Figure 2.	Atomic PDF, G(r), for the neutron scattering profiles of LiAl(ND2)4 (a) before and after heat treatment at (b) 433 K and (c) 673 K [4]. PDF refinement results: observed (black circles), calculated(red line), and residual (blue line) scattering profiles. The reaction process, x in eq. (1), and statistical reliability factors, Rwp, obtained by PDF refinement of the G(r) profiles are shown.

References[1]	R. Janot, J.-B. Eymery and J.-M. Tarascon: J.
Phys. Chem. C 111 (2007) 2335–2340.
[2]	
T. Ono, K. Shimoda, M. Tsubota, S. Kohara,
T. Ichikawa, K. Kojima, M. Tansho, T. Shimizu
and Y. Kojima: J. Phys. Chem. C 115 (2011)
10284–10291.
[3]	
T. Ono, K. Shimoda, M. Tsubota, S. Hino, K.
Kojima, T. Ichikawa and Y. Kojima: J. Alloys
Compd. 506 (2010) 297–301.
[4]	
K. Ikeda, T. Otomo, H. Ohshita, N. Kaneko,
M. Tsubota, K. Suzuya, F. Fujisaki, T. Ono, T.
Yamanaka, K. Shimoda, T. Ichikawa and Y.
Kojima: Mater. Trans. 55 (2014) 1129–1133.

K. Ikeda1,2, T. Otomo1,2,3, H. Ohshita1,2, N. Kaneko1,2, M. Tsubota2, K. Suzuya1, F. Fujisaki3, T. Ono4, T. Yamanaka4,
K. Shimoda5, T. Ichikawa4,5, and Y. Kojima4,51
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3Department
Materials Structure Science, The Graduate University for Advanced Studies; 4Graduate School of Advanced Sciences of Matter, Hiroshima
University, 5Institute for Advanced Materials Research, Hiroshima University

24

Research and Development Highlights

Polymer Brush Layers at Water/Polymer Interfaces Formed bySegregation of Amphiphilic Block Copolymers

polymer brush hence realizes dynamic response
to environmental changes, that is, the block copolymer chains still remaining in bulk are supplied tothe damaged surface immediately if some of copolymers at the brush layer are removed due to physical damage like frictional ware and scratch.
In order to evaluate the density and length of
the brush layers formed at D2O/polymer interfaces,
we performed neutron reflectivity measurements at
SOFIA reflectometer in J-PARC/MLF [5, 6].
2. Results and discussion
Figure 2 shows neutron reflectivity curves atthe D2O/PDMS films containing 20 wt% of PEG-bPDMS (Mn = 2100 - 1000) and at D2O/neat PDMS.
The reflectivity of neat PDMS shows only small fringes that correspond to the total thickness of the filmon quartz substrate, whereas a fringe with a larger
periodicity, ∆q, appeared in the reflectivity of 20 wt%
PEG-PDMS, which indicates the formation of relatively thin but well defined D2O-swollen brush layer.
To analyze the details of the interfacial structures,
we computed the depth profiles of SLD using themulti-layer model. The scattering length density profiles obtained by fitting with box models are shown

Reflectivity

10

Figure 1.	
A schematic picture of the bulk and interfacial
structures of PEG-PDMS in a mixture with PDMS
in contact with air or water.

Soft matter Science

1. Introduction
A layer of polymer chains tethered by one end toa surface is called polymer brush and known to show
various unique properties such as prevention of protein adsorption and anti-fouling activity. These polymer brushes have been usually fabricated by two
methods: polymerization from the surface (“graftingfrom” method) [1] and attaching polymer chain to thesurface either chemically or physically (“grafting-to”
method) [2, 3]. Herein we report a third method tofabricate hydrophilic brush layer utilizing spontaneous segregation of an amphiphilic block copolymer
in a matrix of elastomer to water interface [4].
The surface segregation phenomena of copolymers with surface-active blocks should be usefulfor preparing such a brush layer spontaneously.
Recently, we constructed such self-restoring segregation system using cross-linked poly(dimethyl
siloxane) (PDMS) elastomer for matrix containing
diblock copolymers of poly(ethylene glycol) (PEG)
and PDMS, (PEG-PDMS), as amphiphilic copolymers. In this system, while the hydrophilic block withhigh surface energy avoids air surface it segregatesto cover the interface between hydrophobic PDMS
and water as schematically shown in Figure 1. This

0

10

-1

10

-2

10

-3

10

-4

10

-5

10

-6

neat PDMS
PEG-b-PDMS
2100-1000 20%
fitting
8 9

0.01

2

3

4

5

6 7

q [Å ]-1

Figure 2.	Neutron Reflectivities of sample films containing
no copolymers (neat PDMS) and 20 wt% of PEGb-PDMS (Mn = 2100 - 1000).

Research and Development Highlights

25

Soft matter Sciencefavorable water but also by getting out from unfavorable PDMS via forming the brush layer.

-2

6

4

6

b/V×10 /Å

in Figure 3. The thickness of the brush layer R is
evaluated to be about 15 nm, corresponding to 88%
of the contour length of PEG block Rmax (= 17 nm)with molecular weight of 2100. The brush density
was calculated to be higher than 0.2 chains/nm2
from the profile. Both the thickness and the grafting density indicate that a significantly dense brushlayer is formed by the segregation of amphiphilic
block copolymer, which is comparable to the polymer brush fabricated by the “grafting-from” method.
In order to explain why such a high-density andextremely stretched brush layer is formed by segregation process, we propose a model assuming that(i) energy gain due to the hydration of PEG block isthe driving force for free energy change ∆F by segregation, (ii) stretching entropy loss of PEG chain
competes with (i), and (iii) other effects such as surface energy gain and translational entropy loss bysegregation of copolymers are ignorable. The mostsignificant difference between the conventional
brush and ours, created by segregation, is whether
the grafting density σ is fixed or variable. If a conventional brush chain with fixed σ is placed in water,
it will be swollen and stretched to be saturated ata certain volume fraction of water and the swelling
stops because it gives only stretching entropic loss.
On the other hand, our brush created by segregation of copolymer with variable σ stretches more inwater and gets denser as far as possible with keeping the saturated volume fraction in order to maximize the free energy gain per unit area.
To verify this model, we have calculated ∆F by
the formation of brush layer as a function of elongation R/Rmax and σ. Figure 4 shows the calculated∆F as a function of R/Rmax and σ. This calculation
semiquantitatively supports the idea that brushes
with fixed σ reach only local stable point, whereasa brush created by segregation can be more stretched and denser to come to the global point. Our
brush is more stretched and denser than the prediction of the model (R/Rmax = 0.75 and σ = 0.019), andthis is because enthalpy change is underestimated:
PEG block gains energy not only by getting intoneat PDMS
PEG-b-PDMS
2100-1000 20%

2

0

100

3

200

300

Depth×10 / ÅFigure 3.	Scattering length density profiles at D2O/sample
interfaces obtained by fitting the reflectivity curves.

4

6

b/V×10 /Å-2

6neat PDMS
PEG-b-PDMS
2100-1000 20%

2

0

100

3

200

300

Depth×10 / ÅFigure 4.	Calculated free energy change by hydration andstretching of PEG brush as a function of elongation R/Rmax and grafting density σ.

References[1]	Y. Tsujii et al., Adv. Polym. Sci. 197 (2006) 1.
[2]	A. Halperin et al., P. Adv. Polym. Sci. 100 (1992)31.
[3]	B. Zhao and W. Brittain, J. Prog polym. Sci. 25(2000) 677.
[4]	M. Inutsuka et al., ACS Macro Lett. 2 (2013)265.
[5]	N. L. Yamada et al., Euro. Phys. J. Plus 126(2011) 108.
[6]	K. Mitamura et al., Polymer J. 45 (2013) 100.

M. Inutsuka1, N. L. Yamada2,3, K. Ito1, and H. Yokoyama1
Graduate School of Frontier Sciences, the University of Tokyo; 2Neutron Science Section, Materials and Life Science Division, J-PARC center;3
Institute of Materials Structure Science, KEK

1

26

Research and Development Highlights

Multistep Thickening of Nafion Thin Films in Water Studied
by Optical and Neutron Reflectivity

2. Results and Discussion [1]Figure 1 shows the time dependence of the swelling ratio for Nafion films on silver and SiOx substrates,
respectively, after coming in contact with water. The
swelling ratio here is defined as the value of the film
thickness in water (hw) divided by the thickness (h0)in the dried state. Since the swelling ratio for the film
became larger in water with increasing time, there is
no doubt that water molecules were sorbed into the

1.5
1.4

Swelling ratio

1.3
1.2
1.1
1.0

0

3

6

9

12

15

18

Time・10-3/s

Soft matter Science

1. Introduction
Known for its remarkable conductivity and durability, Nafion is widely used as a proton exchange filmin polymer electrolyte fuel cells (PEFC). Those excellent electrochemical and mechanical properties of
Nafion are associated with the characteristic network
structure of the hydrated water phase. Extensive
studies have revealed that the microstructure in the
Nafion film depends on the swelling ratio. However,it appears to us that most studies conducted so far inthis context are limited to bulk systems. Downsizing
PEFC is one of the interesting developments in thenear future. To accept such a challenge, all components in a PEFC including the polyelectrolyte film
should therefore become smaller and/or thinner.
The physical properties of a polymer film are
generally altered with decreasing thickness for films,
especially when thinner than 100 nm. The effectsof air and substrate interfaces on thin films are undoubtedly responsible for this thickness dependency. Works published in the current literature haveshown that chain dynamics at the air and substrateinterfaces should be enhanced and depressed incomparison with that in the internal region, respectively. This is because the ratio of interfacial area tothe total volume of the film increases markedly withdecreasing film thickness.
In this study, the thickness of thin Nafion films
in water was characterized as a function of time bysurface plasmon resonance (SPR) reflectivity in conjunction with neutron reflectivity (NR) measurements.

Figure 1.	Time dependence of swelling ratio for Nafion films
on silver (red) and SiOx (blue) substrates with an h0of 47 nm and 49 nm, respectively, prior to comingin contact with water. The filled and open symbols
are the data obtained SPR and neutron reflectivity
measurements, respectively.

films. The thin Nafion films thickened in three steps
named here regimes I, II and III. At first, the films asymptotically reached a swelling ratio of 1.05. Then,the films resumed thickening asymptotically up to
1.26. Finally, the swelling ratio reached 1.41. Whilethe characteristic swelling ratio at the border between
different regimes was neither dependent on the substrate species nor the film thickness, the swelling kinetics depended on the type of the substrate.
To examine the aggregation structure of our thin
Nafion films near the substrate interface, NR measurements were conducted. In addition, NR analyses
can verify our results obtained by SPR measurements. Figures 2(a) and (b) show the NR curves for
Nafion films with an h0 of 53 nm supported on silverand quartz substrates respectively in air and D2O atvarious times. Here, D2O was used instead of water.
The solid lines denote the best-fit calculated reflectivity to the experimental ones based on the model(b/V) profiles normal to the interface shown in panels(c) and (d) of Figure 2, respectively. A model (b/V)
profile with a moderately single hydrated interfacial
layer was suitable to the Nafion film on the silver substrate. On the other hand, a model containing such

Research and Development Highlights

27

(b)

100

1

10-2

2

10-4

3

Nafion® on silver

Reflectivity

Reflectivity

(a)

10-6
10-8
0.0

air
D2O 7.0㽢103 s
D2O 1.5㽢104 s

0.1

2

10-4

3

Nafion® on quartz

0.2

1.
2.
3.

10-8

0.3

0.4

q / nm−1

0.5

0.6

0.0

air
D2O 7.0㽢103 s
D2O 1.5㽢104 s

0.1

0.2

D2O

0.3

0.4

0.5

0.6

bound
: waterfree: watersulfonic acid:group

Nafion8(b/V)㽢104 / nm-266transition, was coincident with the asymptotic swelling ratios in regimes I, II and III. Thus, the threestep sorption behavior shown in Figure 1 could be
explained in terms of the structural evolution in theinternal region of the film. Figure 3 shows a modelfor the swelling of a thin Nafion film. It is noteworthy
that the hydrated layer is formed near the substrate.

q / nm−1
Interfacial
layers quartz(d)Nafion8(b/V)㽢104 / nm-2

10-2

silverInterfacial
quartzlayer

D2O

Soft matter Science

ionic cluster

ionic channel

Regime II

Regime III

4

4

0

1

10-6
1.
2.
3.

(c)

2

100

2

D2O 7.0㽢103 s

80

60

20

0

Film thickness / nm

−20

0

D2O 7.0㽢103 s

80

60

20

0

Film thickness / nm

−20

Figure 2.	Neutron reflectivity curves for thin Nafion films
with the original thickness (h0) of 53 nm supportedon (a) silver and (b) quartz substrates in air andD2O. The curves are vertically offset for clarity.
Experimental data sets are shown by symbols,
and the best-fit curves calculated using the model(b/V) profiles shown in (c) and (d) are expressedby solid lines, respectively.

an interfacial layer structure with a total thickness of
ca. 15 nm also gave a better fitting for the film on thequartz substrate. The (b/V) values of two layers in theinterfacial region were lower than that in the internal
region of Nafion. This indicates that H2O was sorbed
in the interfacial region before soaking it into D2O.
The swelling ratios evaluated from NR measurements are also plotted in Figure 2, and are consistent
with the data from the SPR measurements.
It has been accepted that the swelling of bulk
Nafion by water sorption is accompanied by a structural change [2, 3]. In short, the water first binds
to sulfonic acid groups of the side chain portion of
Nafion. When the water content in Nafion increases
further, sphere-like ionic clusters are formed. The
clusters finally connect to one another forming bridges. Interestingly, the swelling ratio for the structural

Regime I
driedswollenTime
Figure 3.	A schematic representation of the structural evolution in a thin Nafion film contacting water.

3. Conclusion
In conclusion, the water absorption kinetics andaggregation states in thin Nafion films were investigated by SPR and neutron reflectivity measurements. The water sorption behavior of thin Nafion
films is divided into three regimes, which could beunderstood by using bulk system concepts, while
its dynamics strongly depends on the substrate dueto the interaction between the substrate and Nafion
and/or the confinement effect.
References[1]	Y. Ogata, D. Kawaguchi, N. L. Yamada, K.
Tanaka, ACS Macro Lett., 36 (2013) 856.
[2]	G. Gebel, J. Lambard, Macromolecules 30,(1997) 7914.
[3]	
K. Schmidt-Rohr, Q. Chen, Nat. Mater. 7,(2008) 75.

Y. Ogata1, D. Kawaguchi2, N. L. Yamada3,4, and K. Tanaka1,5
Department of Applied Chemistry and 2Education Center for Global Leaders in Molecular Systems for Devices, Kyushu University; 3Neutron
Science Section, Materials and Life Science Division, J-PARC center; 4Institute of Materials Structure Science, KEK; 5International Institutefor Carbon-neutral Energy Research (WPI-I2CNER), Kyushu University
1

28

Research and Development Highlights

Precise Evaluation of Angstrom-Ordered Mixed Interfaces
in Solution Processed OLEDs:
Influence on Carrier Transport Characteristics[3]. TFB was spin-coated on the Si substrate andmade insoluble by thermal annealing. CBP:Ir(ppy)3
was spin-coated by using either of two solvents:
1,4-dioxane or cyclopentanone. Furthermore, theinterface of deuterated CBP (CBP-d16) doped withIr(ppy)3 on TFB was investigated to precisely evaluate the interface structure. The evaporated CBPd16:Ir(ppy)3 on TFB was also evaluated. NR measurements were performed using the single frame
mode of the BL16 SOFIA (SOFt Interface Analyzer)
horizontal-type time-of-flight neutron reflectometer (2.0 Å < λ < 8.8 Å) at J-PARC (Japan Proton
Accelerator Research Complex)/MLF (Materials andLife Science Experimental Facility) [4]. Least squares
analysis of the reflectivity profiles was performed using the Motofit reflectometry analysis program [5].
The reflectivity curves of TFB/CBP-d16:Ir(ppy)3and the results of least-square fitting are shownin Fig. 1. Reflectivity curves were well fitted with
two-organic layer models. The interface from theevaporation process was clear. The thicknesses
and SLDs of TFB were the same as those of the
TFB monolayer film. In the interfaces from solution
process, the thicknesses and SLDs of TFB wereincreased from those of the TFB monolayer film.
These show that CBP-d16 and Ir(ppy)3 molecules
mixed to swollen TFB layer. Similar results were obtained in TFB/CBP:Ir(ppy)3 films. Cyclopentanone
has stronger interaction with TFB than 1,4-dioxane.
However, the swollen thicknesses were the same inboth solvents. We assume that cross-linking points
limited the increases of TFB thicknesses. The solvent difference affected the interfacial roughnesses.
Cyclopentanone gave larger interfacial roughness
than 1,4-dioxane. We assume that the interfacialroughness reflect the polymer end-chain. Swellingof polymer end-chain should not be limited by thecross-linking. The SLDs of CBP-d16:Ir(ppy)3 layers
in TFB/ CBP-d16:Ir(ppy)3 were decreased by 3%
from those of CBP-d16:Ir(ppy)3 monolayer films bothin solvents. The CBP-d16 SLD value is almost twice

Research and Development Highlights

Soft matter Science

Organic light-emitting devices (OLEDs) havedistinguishing features like light weight, flexibility,
high power efficiency, being surface light sources,
etc. OLEDs have penetrated next-generation lighting, and the further growth of this market is anticipated [1]. Recently, a solution-process alternative
to ordinary evaporation process has been rapidly
developed to lower the cost. For now, the solutionprocessed OLEDs have inferior characteristics
compared to the evaporation-processed OLEDs.
The formation of clear organic/organic interfaces
is important to improve the characteristics of thesolution-processed OLEDs. However, it is not clear
how the interface from solution process is formed.
Therefore, we investigated the organic/organic interface from solution process.
We used neutron reflectometry (NR) to investigate
the organic/organic interfaces. Layer structure along
depth-direction can be obtained by analyzing the reflectivity curve using Parratt’s formula [2]. Comparedto other methods, such as secondary ion mass spectrometry, NR has the following advantages. NR is a
non-destructive method, therefore there is no artifact
created by destruction of the sample. Also, NR has
intrinsic neutron wavelength-ordered resolution. The
neutron wavelength used in experiment is angstromorder, therefore depth-direction analysis with angstrom-ordered resolution is possible. X-ray reflectometry (XRR) also has these advantages. However,
the investigation of the organic/organic interface by
XRR is difficult, because the scattering length densities (SLDs) of organic layer for X-ray are close values
among almost organic aromatic compounds. In contrast, the differences of the SLDs for NR can be enhanced by deuteration of material consisting of one
layer (D/H contrast method).
We investigated the organic/organic interface of
deuterated 4,4’-bis(N-carbazolyl) biphenyl (CBP)
doped with fac-tris(2-phenylpyridyl) iridium(III)(Ir(ppy)3) on hole transport polymer poly(9,9-dioctylfluorene-co-N-(4-butylphenyl)-diphenylamine) (TFB)

29

Soft matter Science
Figure 1.	Reflectivity curves and SLD profiles. The reflectivity scale corresponds to the profile for Si/TFB/
CBP-d16:Ir(ppy)3(evaporation). Other plots are offset for clarity.

the SLD of Ir(ppy)3. This indicates that CBP-d16 ismore mixed to swollen TFB layer than Ir(ppy)3.
Hole only devices (HODs) were fabricated to investigate the effect of these interface structures on thecharacteristics of hole transport abilities. HODs with astructure of [ITO/PEDOT:PSS (40 nm)/TFB (20 nm)/
CBP:12 wt% Ir(ppy)3 (40 nm)/α-NPD (40 nm)/MoO3(5 nm)/Al (100 nm)] were fabricated, where the
α-NPD, MoO3, and Al layers were formed by evaporation. CBP:12 wt% Ir(ppy)3 layers were evaporated
or spin-coated by using either of 1,4-dioxane or cyclopentanone. The driving voltage of the evaporated
device was lower than that of the spin-coated devices. Also, the driving voltage of the spin-coated device
using 1,4-dioxane was lower than that of the spincoated device using cyclopentanone. Fig. 2 showsthe energy diagram of HOD with solution-processed

CBP:12 wt% Ir(ppy)3 layer. We assume that thecauses for increase of the driving voltages are the decrease of the triphenyl amine density and hole trapping by HOMO level of Ir(ppy)3 in mixed layer.
In conclusion, we investigated the TFB/CBPd16:Ir(ppy)3 interfaces from solution processes
by NR. We found swollen TFB layer and CBPd16:Ir(ppy)3 mixing to swollen TFB layer. These interfacial mixings affected the device characteristics. The precise evaluation of the organic/organicinterfaces and improvement of interfacial formation
method are important to enhance the characteristics of solution-processed OLEDs.
We would like to thank the “Strategic Promotion of
Innovative R&D Program” and the “Japan Regional
Innovation Strategy Program by Excellence” of Japan
Science and Technology Agency (JST) for their financial support. The NR experiment was approvedby the Neutron Science Proposal Review Committeeof J-PARC/MLF (Proposal No. 2012B0089) and supported by the Inter-University Research Program on
Neutron Scattering of IMSS, KEK.

Figure 2. Energy diagram of solution processed HODs.

References[1]	H. Sasabe and J. Kido, J. Mater. Chem. C. 1,
1699 (2013).
[2]	R.-J. Roe, Methods of X-ray and Neutron
Scattering in Polymer Science, Oxford University
Press, New York, America, (2000).
[3]	S. Ohisa et al., Adv. Mater. Interfaces, in printing(DOI: 10.1002/admi.201400097).
[4]	K. Mitamura et al., Polym. J. 45, 100 (2013).
[5]	A. Nelson, J. Phys.: Conf. Ser. 251, 012094 (2010).

S. Ohisa1, G. Matsuba1, N. L. Yamada2,3, Y.-J. Pu1, H. Sasabe1, and J. Kido1
1
Graduate School of Science and Engineering, Yamagata University; 2Neutron Science Section, Materials and Life Science Division, J-PARC
center; 3Institute of Materials Structure Science, KEK

30

Research and Development Highlights

SANS and SAXS Studies on Aggregates Properties ofa Novel Sugar-Type Surfactant in Aqueous Solution

Figure 1.	Chemical structure of amphiphilic multi-sugar typesurfactant (C12-mGEMA) with a hexadecyl chain ina terminal group and multi-sugar chains. GEMA isa glucosyloxyethyl methacrylate.

2. Experimental
C12-mGEMA molecules with varying number ofsugar from 3.0 to 7.1 were systematically synthesized according to a procedure described in the
recent report [1]. After synthesis, we confirmed thechemical structure, including the number of sugar,
by employing 1H-NMR and elemental analysis. The
C12-mGEMA solutions were prepared by dissolving 25 mg/ml of C12-mGEMA lyophilized powder
in an aqueous solution. The pure D2O (Cambridge
Isotope Laboratories Inc., Andover, MA) was used
for SANS measurements. SANS experiments were
performed using the TAIKAN instrument installedon the BL15 beamline at the MLF, J-PARC (Tokai,
Japan). The covered Q range was 0.015 – 3.0 Å−1
in one measurement, where Q is defined by Q =4πsin(θ/2)/λ (λ and θ represent the wavelength andthe scattering angle, respectively). The exposure
time for each sample was 3 hours. SAXS experiments were performed using the SAXS spectrometer installed on BL10C beamline at the Photon
Factory, KEK (Tsukuba, Japan). The sample-todetector distances were 1 m, and the X-ray wavelength was 1.488 Å. The covered Q-range was 0.01
– 0.3 Å−1. The exposure times were 10 minutes.
SANS and SAXS measurements were performed at
an ambient temperature.

Soft matter Science

1. Introduction
Recently, we successfully synthesized a novel
sugar-type surfactant (C12-mGEMA; GEMA is a glucosyloxyethyl methacrylate) with a dodecyl chain ina terminal group involving multi-sugar chains (m:the number of sugar) [1]. Figure 1 shows the chemical structure of C12-mGEMA. By employing surface
tension measurements, C12-mGEMA was shown to
exhibit a higher efficiency in lowering the surface
tension of water. In addition, we found that C12mGEMA effectively acts as a stabilizer for synthesizing metal nanoparticles. However, no information
was gathered on the aggregate structure formed by
C12-mGEMA in an aqueous solution. In this study,
by using small-angle neutron scattering (SANS)
and small-angle X-ray scattering (SAXS), we investigated the meso-scale aggregate behavior of theC12-mGEMA in an aqueous solution depending on
the number of sugar. The combined use of SANS
and SAXS is one of the most effective techniques toquantitatively reveal aggregates of amphiphilic molecules in solutions.

3. Result and Discussions
Figures 2(a) and 2(b) show SANS and SAXS
profiles for C12-mGEMA solutions depending on thenumber of sugar (m). SANS profiles were decreased
drastically at around Q = 0.05 Å−1. In contrast, SAXS
profiles exhibited a bell-shaped peak profile in the
Q-range of 0.15 Å−1 < Q < 0.3 Å−1. The SAXS profiles consistently differed from the SANS results. In
the case of SAXS for a micellar structure formedby amphiphilic molecules in water, the observed
peak profile was attributed to greater difference inthe scattering length density (so-called contrast) between hydrophilic and hydrophobic portions. On the

Research and Development Highlights

31

Soft matter Science

Figure 2.	(a) SANS and (b) SAXS profiles for C12-mGEMA in an aqueous solution with varying the number of sugar (m).
Solid lines are the best fitted theoretical scattering curves. Each profile is vertically shifted to avoid overlapping.

other hand, in the case of SANS, when D2O wasused as a solvent, the contrast for the neutrons between the hydrophilic and the hydrophobic portions
was lower than that between D2O and amphiphilicmolecules. Therefore, the peak profile was absent
in the SANS profiles.
In Figure 2(a), in the Q-range of Q > 0.1 Å−1,
the SANS profile showed power law behavior I(Q)
~ Q−a. The power law exponent (a) was decreased
from 4.1 to 1.7 with increasing the number of sugar. In the SAXS profiles [shown in Figure 2(b)], thepeak profile in the Q-range of 0.1 Å−1 < Q < 0.4 Å−1
gradually became broader.
To determine the structural parameters quantitatively, model-fitting analysis was performed on
both the SANS and the SAXS profiles using a theoretical scattering function given by a product of theform factor P(Q) and the structure factor S(Q). We

employed a core-shell prolate ellipsoid model forP(Q) and a hard sphere model given by the PercusYevick approximation [2]. All best-fit theoreticalscattering curves are shown in Figures 2(a) and2(b). The theoretical scattering curves appropriately
agree with all experimental results. By increasing
the number of sugar, the overall radius was slightly
decreased from 1.9 to 1.4 nm, whereas the overall axis ratio was significantly increased from 1.6 to
4.2. The results suggest that the shape of micelles
formed by C12-mGEMA in an aqueous solutionchange from a spherical shape to an ellipsoid byincreasing the number of sugar.
References[1] Yoshimura et al., in preparation[2]	J. Percus and G. J. Yevick, J. Phys. ReV. 110,
1 (1959).

K. Akutsu1, H. Iwase1, Y. Nakatani2, and T. Yoshimura2
Neutron R&D Division, CROSS-Tokai; 2Research Group of Chemistry, Division of Natural Sciences, Nara Women’s University

1

32

Research and Development Highlights

Neutron Brillouin Scattering of Hydrated β-Lactoglobulin

whether or not the collective dynamics changes
around the dynamic transition temperature (~ 220 K;
the pico-second dynamics measurements revealed
that the mean square displacement of some hydrated
proteins increase remarkably at this temperature [5]).
2. Experimental
β-lactoglobline powder (SIGMA-ALDRICH) wasused without further purification. The powder was
dissolved in D2O and lyophilized. The process was
repeated three times to exchange labile hydrogensof the protein with deuterons. Then the dry protein
powder was kept in a desiccator with saturated vapor of D2O. The D2O absorbed protein powder (withhydration level of 0.4) was sealed into a rectangle
cell made of aluminum under helium atmosphere.
The inner dimensions of the cell were 30 × 30 ×
9.5 mm3. Indium wire was used for sealing. The
cell was stored in the vacuum chamber of the HRC
spectrometer. A cryostat equipped in BL12 controlled the temperature of the sample.
Phonon excitations in the hydrated protein were
measured at T = 300 K with Ei = 102 meV and ΔE= 2.0 meV. The data were accumulated typically for
2 days at each temperature.

Life Science

1. Introduction
The dynamics of biomolecules in water comprises not only micro- and millisecond-scale formationalchanges (e.g. domain motion of protein) but alsopico- and femto-second-scale fluctuations. The former is directly related to the biological activity and/or function of protein (e.g. molecular recognition
process), whereas the latter is concerned with the
diffusive and vibrational motions of biomolecules
and the surrounding water molecules. Hydrationof biomolecules directly perturbs the latter dynamics to induce the former dynamics easily due tothe conformational flexibilities of the biomolecules.
Therefore, investigation of pico- and femto-second
dynamics is highly needed for understanding a possible mechanism of the biological functions and theactivities of biomolecules in water.
Many elastic and quasi-elastic neutron scattering
measurements for hydrated proteins have revealed
that the motions of hydrated proteins and hydrationwater change drastically with the hydration level andtemperature [1, 2]. These dynamics are mainly reflected on the diffusive motion of protein atoms andhydration water molecules because of the energy
resolution of micro-eV order. On the other hand, millieV dynamics corresponding to collective vibrationalmotion on the femto-second time scale is observed byinelastic X-ray scattering and neutron Brillouin scattering (NBS). There are few studies on the collective
dynamics of hydrated proteins because of the difficulty of the measurements. Previously, we performed
inelastic X-ray scattering of hydrated β-lactoglobulin
at a few hydration levels [3]. The collective dynamics of hydrated proteins also changes depending on
the hydration level. Orrechini et al. measured NBS of
hydrated ribonuclease at room temperature [4] andrevealed that the NBS spectra reflect the collective
dynamics of hydration water of the protein.
In the present study, NBS of hydrated
β-lactoglobline at 180 and 298 K was measured on
the HRC spectrometer at BL12 of MLF to investigate

3. Results
Figure 1 shows the scattering intensity of hydrated β-lactoglobline at 298 K. The spectrum showedshoulders due to symmetrical excitation peaks and a
resolution-limited elastic peak. The excitation peaks
were fitted with a damped harmonic oscillator scattering function convoluted with the resolution width
multiplied by a temperature factor (Bose-Einstein
factor). The peak positions Ep(Q) were determined
as a function of Q. The present analysis is identicalto that for D2O measured previously at BL12 [6].
In Fig. 2, the Q dependence of the Ep(Q) values is shown at 180 and 298 K. At both temperatures, a dispersion relation is found. The slope indicates the velocity of the high-frequency sound.

Research and Development Highlights

33

101
298 K

Intensity

100
10-1
10-2
10-3

-10

0
E / meV10

Figure 1.	The NBS spectrum of hydrated β-lactoglobulin at
a hydration level = 0.4 as a function of excitationenergy E at Q = 5.0 nm−1 at 298 K. The solid line
indicates the DHO fitting results.

20
180 K
10

Ep / meVLife Science

0
298 K

10

0
0

2

4
6
-1
Q / nm8

10

Figure 2.	The dispersion relation between the inelastic excitation peak Ep(Q) and the momentum transfer Q
for hydrated β-lactoglobulin at a hydration level =0.4 at 180 K and 298 K. The open circles indicate
the NBS results and the filled circles are the IXS
ones [3]. The solid lines show the least-squares
fits in the NBS results.

These values at 180 and 298 K are 2430 ± 80 and
2460 ± 110 ms-1, respectively. The high-frequency
sound velocity at 298 K is almost the same as thatat 180 K within the experimental errors. That is, thedynamic transition at ~ 220 K is not very remarkablein femto-second collective dynamics of the hydrated
protein. This is consistent with the results of the IXS

measurement, where the high-frequency sound of
hydrated lysozyme does not change drastically inthe temperature range between 300 and 190 K [7].
The high-frequency sound velocity at 298 K in
the present study is a little smaller than that obtained
from the IXS experiments [3]. For neutron scattering,the contribution from deuterons is more dominant.
The difference in the high-frequency sound velocity
might be influenced by hydration of heavy water.
4. Future Plans
Femto-second dynamics observed with inelastic scattering is sensitive to atomic potentials which
determine protein structure and interaction with hydration water. Molecular dynamics (MD) simulationsof proteins require more realistic atomic potentials.
The femto-second dynamics data can help to validate experimentally the atomic potentials using the
MD simulations. Neutron scattering can provide information on the individual parts of proteins by using the H/D substitution technique. The dynamics ofactive sites of proteins is selectively obtained whenpartially deuterium labeled proteins are available.
To connect function and activities of proteins withfemto-second dynamics, investigation of different
types of proteins is necessary.
References[1]	“Workshop on Hydration Processes in Biology:
Theoretical and Experimental Approaches”(M.C. Bellissent-Funel, ed.), IOS Press, 1998.
[2]	“Water: The Forgotten Biological Molecule” (D.
Le Bihan, H. Fukuyama, eds.), Pan Stanford
Publishing, 2011.
[3]	K. Yoshida et al., J. Chem. Phys. 133 (2010)
134501-1-7.
[4]	A. Orecchini et al., J. Am. Chem. Soc. 131(2009) 4664–4669.
[5]	W. Doster et al., Nature 337 (1989) 754-756.
[6]	S. Itoh et al., J. Phys: Conference Series 502(2014) 012043-1-5.
[7]	Z. Wang et al., J. Phys. Chem. B 117 (2013)
1186–1195.

K. Yoshida1, T. Yamaguchi1, D. Kawana2, T. Yokoo3,4, and S. Itoh3,4Facluty of Science, Fukuoka University; 2The Institute for Solid State Physics, The University of Tokyo; 3Neutron Science Section, Materials
and Life Science Division, J-PARC center; 4Institute of Materials Structure Science, KEK

1

34

Research and Development Highlights

Inelastic Neutron Scattering Study inMultiferroic Compound NdFe3(11BO3)4

Figure 1.	The crystal structure (a) and magnetic structure(b) of NdFe3(BO3)4 (hexagonal, space-group R32).

2. Experimental Details
Single crystals of NdFe3(11BO3)4 were grown by
a flux method. 22 pieces of single crystals werecoaligned by using transmission X-ray Laue camera.
The total mass of the crystals was 2.1 g. The inelastic neutron scattering experiment was performed at
the High Resolution Chopper (HRC) spectrometer
installed in MLF/J-PARC. The incident energy Ei wasset to 11.46 meV. Soller collimator with a divergenceangle of 1.5° was installed in front of the sample
to eliminate the direct beam contamination, and a
200 Hz Fermi chopper, "S", was used to obtain highflux neutrons. The single crystals were mounted sothat a*c* plane was horizontal. We set the sample
temperature at 15 K in the commensurate orderedphase. The a*-axis was initially parallel to the incident
neutron beam and the crystals were rotated counterclockwise by 70 degrees with steps of 2 degrees.

Magnetism &Strongly Correlated Systems

1. Introduction
Symmetry breaking of time reversal and space
inversion allows spontaneous order both in magnetism and dielectricity. The enhanced simultaneousorder, multiferroics, has been extensively studied
since the discovery of its experimental realization in
the perovskite manganite TbMnO3. The rare-earth
iron borates RFe3(BO3)4 (R = rare-earth metal) area new family of multiferroic compounds. The crystal
structure of NdFe3(BO3)4 is shown in Fig. 1(a). Fe3+
ions carry S = 5/2 spins and Nd3+ ion carry J = 9/2
moments. FeO6 octahedra form spiral chains withthree-fold rotational symmetry along the crystallographic c-axis. Bulk property studies reported thatan antiferromagnetic order of easy-plane type andspontaneous electric polarization simultaneously
appeared at TN = 30 K, and that the electric polarization was enhanced by applying magnetic field[1-3]. Neutron diffraction [4] revealed collinear magnetic order in the intermediate temperature range
TN ≥ T ≥ TIC = 13.5 K in Fig. 1(b). Below TIC incommensurate magnetic order appeared. In spite of accumulative studies on static properties, microscopic
dynamics in wide energy wave number space has
not been reported so far. In this report we study
magnetic excitation by means of inelastic neutron
scattering technique to identify the magnetic modelin the multiferroic compound NdFe3(11BO3)4.

3. Experimental results
We collected inelastic neutron spectrum, where
well-defined excitations were observed. We extracted constant Q cuts from the data, fitted the data by
Gaussian function, and plot the peak energies foreach cut by filled circles as shown in Figs. 2(a) and(b). Here Q = (0, 0, -1.5) is the magnetic Bragg peak
position. A dispersive excitation with band energy of
5.5 meV along the c* direction was observed. An anisotropy gap with magnitude of about 0.5 meV wasobserved at Q = (0, 0, -1.5), which was consistent
with a previous ESR study [5]. The excitation is ascribed to Fe3+ centered spin wave excitation which
will be explained later. A flat excitation is observed at
1.3 meV. This mode is explained by the energy splitof the Kramers doublet of the Nd3+ ion due to theexchange interaction with the Fe3+ ion. Anti-crossing
is observed between the dispersive and non-dispersive modes, which means the existence of interaction between Fe3+ and Nd3+ ions. The magnetic excitations are more dispersive along the c* directionin Fig. 2(a) than the a* direction in Fig. 2(b), which

Research and Development Highlights

35

(a)

8

E (meV)

6
4
2
0
-2.0

(b)

-1.5

-1.0

-0.5

(0, 0, L)

0.0

8

E (meV)

6
4
2
0
-1.5

-1.0

-0.5

0.0

0.5

1.0

(H, 0, -1.5)

1.5

Figure 2.	(a) Magnetic excitation along the c*-direction. (b)Magnetic excitation along the a*-direction.

Magnetism &Strongly Correlated Systems

means that the magnetic interaction along the c direction, i.e., the Fe3+ chain direction is dominant.
4. Analysis
In order to identify the magnetic model of
NdFe3(11BO3)4, we performed spin wave calculationby using a Holstein-Primakoff transformation [6].
The minimal model of the Hamiltonian is as follows:
H= − ∑ J1Si⋅Sj − ∑ J2Si⋅Sj
n.n

n.n.n

( ) −∑h J− ∑ J3Si⋅Jk − ∑ Di Si

z

n.n

i

2

eff

z

k

k

The first term is the exchange interaction between Fe
spins along the inchain direction and the second termis that along the interchain direction, which leads to thedispersion along the c*- and a*-directions, respectively.
The third term is the interaction between Fe3+ and Nd3+
ions, which induces the anti-crossing of the spin waveof Fe3+ ions and the crystal field of Nd3+ ions. The forthterm is the single ion anisotropy of Fe3+ ions. The lastterm is the energy split of Kramers doublet of Nd3+ ionsdue to the staggered field of Fe3+ ions.
Fit to the data is indicated by the solid curves in
Figs. 2(a) and (b). The obtained parameters are J1= 0.48 meV, J2 = 0.050 meV, J3 = 0.027 meV, D =0.005 meV, and heff = 0.135 meV. The reasonable fit to
the data means that the dispersive excitation is dominantly explained by weakly coupled Fe3+ spin chains.
The flat mode is dominated by the Zeeman split of the
Kramers doublet of Nd3+ crystal field. Anti-crossing between Fe3+ spin wave and Nd3+ crystal field is ascribedto the interaction between Fe3+ and Nd3+ moments.
5. Conclusion
We measured the inelastic neutron spectrum inthe multiferroic compound NdFe3(11BO3)4 by rotating the single crystals at the HRC spectrometer. The
observed well-defined excitations were reasonably
explained by spin-wave calculation based on our
minimal magnetic model.
References[1]	N. Tristan, R. Klingeler, C. Hess, B. Büchner, E.
Popova, I. A. Gudim, and L. N. Bezmaternykh,
J. Magn. Magn. Mater. 316, E621 (2007).
[2]	A. M. Kadomtseva, Yu. F. Popov, G. P. Vorob’ev,
A. P. Pyatakov, S. S. Krotov, K. I. Kamilov, V.
Yu. Ivanov, A. A. Mukhin, A. K. Zvezdin, A. M.
Kuz’menko, L. N. Bezmaternykh, I. A. Gudim, andV. L. Temerov, Low Temp. Phys. 36, 511 (2010).
[3]	A. K. Zvezdin, G. P. Vorob’ev, A. M. Kadomtseva,
Yu. F. Popov, A. P. Pyatakov, L. N. Bezmaternykh
A. V. Kuvardin, and E. A. Popova, JETP Lett. 83,
11 (2006).
[4]	P. Fischer, V. Pomjakushi, D. Sheptyakov, L.
Keller M. Janoschek, B. Roessli, J. Schefer,
G. Petrakovskii, L. Bezmaternikh, V. Temerov
and D. Velikonov, J. Phys.:Condens. Matter 18,
7975 (2006).
[5]	A. M. Kuz’menko, A. A. Mukhin, V. Yu. Ivanov,A. M. Kadomtseva, and L. N. Bezaternykh,
JETP Lett. 96, 294 (2011).
[6]	Albert W. Sáenz, Phys. Rev. 125, 6 (1961).

S. Hayashida1, M. Soda1, K. Ohgushi1, S. Itoh2,3, T. Yokoo2,3, and T. Masuda1
1
The Institute for Solid State Physics, The University of Tokyo; 2Neutron Science Section, Materials and Life Science Division, J-PARC center;3
Institute of Materials Structure Science, KEK

36

Research and Development Highlights

Spin-Wave Dispersion in Nd-Fe-B Permanent Magnets
Observed by Neutron Brillouin Scattering

2. Spin-wave dispersion measurement
However, measuring the exchange stiffness constant is rather difficult. The simplest determinationof exchange stiffness constant from the Curie temperature has generally led to the lower bound forthe exchange stiffness constant, because the molecular field theory omits the low-energy spin-wave
excitations. Therefore, the exchange stiffness constant derived from the spin-wave stiffness constanteither with spin-wave dispersion measurements ismore realistic.

The best way to measure the exchange stiffness
constant is derived from the spin-wave stiffness
in the low-energy spin-wave dispersion, because
the energy of the long-wavelength spin wave isassociated with a gradual twist in the magnetization. Inelastic neutron scattering (INS) is the mostdirect method to determine the spin-wave dispersion, however, a large single-crystalline sample isneeded for INS and the measurements for either
polycrystalline or powder samples are difficult.
3. Neutron Brillouin scattering (NBS)
We propose the use of neutron Brillouin scattering (NBS) with sub-eV pulsed neutrons to determine
the spin-wave dispersion in polycrystalline Nd-Fe-B
magnets. NBS is an advantageous method for observing coherent excitations in non-single-crystalline materials. The dynamic structure factor for ferromagnetic spin-waves in polycrystalline samples
was averaged and the scattering intensities weredetected in the forward direction with a momentum transfer (Q) near 0, and were rapidly decreasing with an increasing Q. Neutrons with an incident
energy (Ei) in the sub-eV region are necessary tomeasure meV-range low-energy excitations withhigh energy resolution. Furthermore, small scattering angles are required to detect the scattered neutrons. Recently, efforts in realizing the experimental
conditions with the NBS method have been madewith a high-resolution chopper spectrometer (HRC)
installed at J-PARC/MLF [2, 3, 4].

Magnetism &Strongly Correlated Systems

1. Introduction
The permanent magnets with high coercivity
have been under intensive study because of theirapplication in high-power motors used in hybrid andelectric vehicles. The Nd-Fe-B magnet is the mostcommonly used magnet with both high saturation
magnetization and magneto-crystalline anisotropy.
For understanding the coercivity mechanism, it isindispensable to know the intrinsic magnetic properties of magnetic materials.
Spin-wave dispersion in magnetic materials isvery important as it provides a microscopic viewpoint for the phenomenological magnetic parameters. Along with the saturation magnetization,
Curie temperature and magnetostatic energy, magnetocrystalline anisotropy (K1) and exchange stiffness constant (A) determine a wide range of magnetic properties in magnetic materials such as thedomain-wall width, domain-wall energy, exchange
length, hardness parameter, single-domain radius
and anisotropy field.
Among the phenomenological magnetic parameters, the exchange stiffness constant is of particular importance in the magnetization reversal process as it measures the strength of the exchangeinteraction between the magnetic moments in amagnet. Thus, the exchange stiffness constant describes the non-uniform magnetization reversal process in a magnet.

4. NBS experiments at HRC in J-PARC/MLF
In the NBS function at HRC, a monochromatic
incident neutron beam with energy Ei illuminatedthe sample and the energy transfer of the scatteredneutrons was determined using the time-of-flightmethod. For the NBS measurements, scatteredneutrons were collected with the two-dimensionalbank of the PSD array at low scattering angles ϕ =0.5 − 2.8°.

Research and Development Highlights

37

A polycrystalline Nd-Fe-B strip-cast sample wasused for the NBS experiment. Natural boron was
substituted for 11B to reduce neutron absorption.
The energy of the incident neutron beam was set
at 257 meV with an energy bandwidth of 5.7 meV.
NBS measurements were performed at sample
temperatures of 300 K and 6 K.

Magnetism &Strongly Correlated Systems

5.	Exchange stiffness constant determined by
NBS
Figure 1 shows the spin-wave dispersion curve
for an Nd-Fe-B magnet measured using NBS. We
observed quadratic spin-wave dispersion, which isin good agreement with the previous inelastic neutron scattering results for a single crystal [5, 6].
The low-energy spin-wave dispersion in the limitof the small wave-vectors is described as E(Q) = E0
+ Dsw Q2, where E0 is the energy gap at Q = 0 and
Dsw is the spin-wave stiffness constant. In NBS, Q
values around 0 could not be accessed. Thus, E0 =2.0 meV was obtained from the bulk value of K1 =4.5 MJ/m3 [7]. The spin-wave stiffness constant Dsw
was found by fitting the spin-wave dispersion. From
15

E (meV)

10

5

HRC(polycrystal)
Mayer et al. 295K
Mayer et al. 6K(single crystal)2
fit to E(Q)=E0+DQ

E = 5 meV

Nd2Fe14B
T = 300 K
Ei = 250 meV

0
0.0

0.1

0.2

0.3

0.4

-1

Q (A )
Figure 1.	Spin-wave dispersion curves for the Nd-Fe-B magnet measured using NBS. The blue dot indicates thepeak position observed using NBS. The blue line
shows the fit of the experimental data to a quadratic
equation. The red line shows the detection limit of thepresent NBS set up with the detector bank at 0.64°.

the fitting we were able to determine Dsw = 100.0 ±4.9 meVÅ2. From the spin-wave dispersion measurements we determined the exchange stiffness
constant, A of 6.6 ± 0.3 pJ/m. This value is comparable to the reported values of 7.3 − 12.5 pJ/m [1] andthe exchange stiffness constant measured by NBS
was considered reliable, as NBS is a direct methodin accessing the spin-wave properties of magnets.
This work was supported in part by the Elements
Strategy Initiative Center for Magnetic Materials(ESICMM) under the outsourcing project of MEXT.
The sample fabrication was performed in part under the Magnetic Materials for High-Efficient Motors(MagHEM) project.
References[1]	
H. Kronmüller and M. Fähnle, “Micromagnetismand the Microstructure of Ferromagnetic Solids”,
Cambridge University Press (2003).
[2]	S. Itoh, T. Yokoo, S. Satoh, S. Yano, D. Kawana,J. Suzuki, and T. J. Sato, Nucl. Instr. Meth.
Phys. Res. A 631, 90 (2011).
[3]	S. Itoh, Y. Endoh, D. Kawana, Y. Kaneko, Y.
Tokura, and M. Fujita, J. Phys. Soc. Jpn. 82,
043001 (2013).
[4]	S. Itoh, T. Yokoo, D. Kawana, and Y. Endoh, J.
Phys. Soc. Jpn. 82, SA034 (2013).
[5]	H. M. Mayer, M. Steiner, N. Stüβer, H. Weinfurter,
K. Kakurai, B. Dorner, P. A. Lindgård, K. N.
Clausen, S. Hock, and W. Rodewalde, J. Magn.
Magn. Mat. 97, 210 (1991).
[6]	H. M. Mayer, M. Steiner, N. Stüβer, H. Weinfurter,
B. Dorner, P. A. Lindgård, K. N. Clausen, S.
Hock, R. Verhoef, J. Magn. Magn. Mat. 104-107,
1295 (1992).
[7]	S. Hirosawa, Y. Matsuura, H. Yamamoto, S.
Fujimura, M. Sagawa, and H. Yamauchi, J.
Appl. Phys. 59, 873 (1986).
[8]	K. Ono, N. Inami, K. Saito, Y. Takeichi, M. Yano,
T. Shoji, A. Manabe, A. Kato, Y. Kaneko, D.
Kawana, T. Yokoo, and S. Itoh, J. Appl. Phys.
115, 17A714 (2014).

K. Ono1, N. Inami1, K. Saito1, Y. Takeichi1, M. Yano2, T. Shoji2, A. Manabe2, A. Kato2, Y. Kaneko3, D. Kawana1, T. Yokoo1,4,and S. Itoh1,41Institute of Materials Structure Science, KEK; 2TOYOTA Motor Corporation; 3Toyota Central R&D Labs. Inc.; 4Neutron Science Section,
Materials and Life Science Division, J-PARC center

38

Research and Development Highlights

Doping-Evolution of High-Energy Spin Excitationin the Electron-Doped Pr1.4−xLa0.6CexCuO4

2. Experimental details
High-energy inelastic neutron measurements werecarried out on assembled single crystals of x = 0, 0.08
and 0.18 at the chopper spectrometer 4SEASONS(BL01). All samples used in this study are as-grown
and non-superconducting crystal. To observe the spin
excitations in wide energy and momentum spaces

with the high efficiency, we applied a multi-Ei method,which was developed in J-PARC [5]. The samples
were set so that the crystallographic c-axis was parallel to the incident neutron beam and cooled down to 6
K by a closed-cycle refrigerator.
3. Results and discussion
Fig. 1 shows the intensity contour map for themagnetic excitation after subtracting the non-magnetic background. Well-defined spin-wave excitation
emerging from h = 0.5 was observed in the x = 0
sample. The zone boundary energy determined fromthe dispersion was ~ 320 meV. The intensity lying at~ 100 meV in a wide momentum range corresponds
to a crystal field excitation from Pr3+ ion. As seen in
the figure, the high-energy excitation shows a drastic doping evolution, that is, the magnetic excitation
gets steeper with increasing the Ce concentration.
This trend can be clearly seen in the constant-energy spectrum sliced at 280 meV along h-direction
through (0.5, 0.5) reciprocal position (Fig. 2). The
magnetic intensity in x = 0 shows peaks at the h =0 and ±1, while the main peaks locate at h = ±0.5
in x = 0.18. This shift of the peak position from thezone-center to the zone-boundary is consistent withthe elongation of the magnetic excitation toward thehigh-energy region. This trend is in stark contrast
to a negligible doping dependence of high-energy spin excitation in the hole-doped LSCO. Thus,
electron-hole asymmetry exists in the spin excitation against doping. We note that the elongation ofmagnetic excitation spectrum with electron-doping
was observed by our recent resonant inelastic X-ray
scattering measurement [6]. Such doping evolution
would be difficult to understand within a simple model based on the localized spin picture, which takes
only the nearest neighbor spin interaction into account. In the La2CuO4 [7], the existence of higher
term exchange interaction is reported. More microscopic consideration is required to clarify the originof anomalous doping evolution of spin excitation.

Research and Development Highlights

Magnetism &Strongly Correlated Systems

1. Introduction
In the research of high-transition-temperature superconductivity, the evolution of the spin excitation
with doping is a fascinating and long-standing issue.
It is well known that the conventional spin-wave excitation in Mott insulator La2CuO4 or YBa2Cu3O6 turns
into the hourglass shaped excitation by the holedoping [1,2]. In the low-energy region, the spin excitation exhibits the incommensurate character withthe propagation vector parallel to the CuO bonding
direction in the superconducting (SC) phase, while
the high-energy excitation remains spin-wave-like
dispersion. Such a distinct doping-dependence ofspin excitations separated by the energy is one ofkeys to understand the role of magnetism in themechanism of superconductivity. In contrast to theprogressive research in the hole-doped system, lessis known about the entire spin excitation in the electron-doped cuprates. Fujita [3] and Wilson [4] separately observed the spin excitation up to ~ 200 meV
in the SC sample and clarified a steeper excitation
along the energy direction than in the undoped compound. This result suggests an increase in the zone
boundary energy by the electron-doping, unlike thedoping-independent high-energy dispersion in thehole-doped system. However, even in the parent
compound, measurement of high-energy spin excitation up to the zone boundary is still missing. Thus,in order to confirm the electon-doping dependence ofspin excitation and gain an insight into the electronhole symmetry in the spin correlation, we performed
pulsed neutron-scattering measurement on a seriesof Pr1.4−xLa0.6CexCuO4 with different x.

39

Magnetism &Strongly Correlated Systems

Figure 2.	(Upper figure) Image of the doping evolution of spin
excitation, which is suggested from the present neutron scattering experiment. (Lower figure) Constantenergy spectrum in the Pr1.4−xLa0.6CexCuO4 with x= 0 (blue), 0.08 (pink) and 0.18 (green) sliced at
280 meV.

Figure 1.	Spin excitation spectrum in the Pr1.4−xLa0.6CexCuO4
with (a) x = 0, (b) 0.08 and (c) 0.18. To enhance thehigh energy excitation, the value of energy transfer was multiplied to the intensity after subtracting
the background. The flat band around 100 meV isa crystal field excitation from Pr3+ ion.

4. Summary
We preformed neutron scattering measurementon the as-grown single crystal of Pr1.4−xLa0.6CexCuO4
to evaluate the doping evolution of spin excitation in
the electron-doped system. We found the elongation of spin excitation against doping, which is quite
different from the negligible doping effect seen in

the hole-doped system. Therefore, electron-holeasymmetry exists in the observed spin excitation
against the doping.
References[1]	J. M. Tranquada et al., Nature 375, 531 (2004).
[2]	S. M. Hayden et al., Nature 375, 534 (2004).
[3]	M. Fujita et al., J. Phys. Soc. Jpn., 75, 093704(2006).
[4]	Stephen D. Wilson et al., PRL 96, 157001(2006).
[5]	M. Nakamura et al., J. Phys. Soc. Jpn., 78,
093002 (2009).
[6]	K. Ishii et al., Nature Comm. 5, 3714 (2014).
[7]	R. Coldea et al., Phys. Rev. Lett. 86, 5377
(2001).

M. Fujita1, K. Ishii2, K. Tsutsumi3, K. Sato3, and R. Kajimoto4
Institute for Materials Research, Tohoku University; 2Quntum Beam Science Center, Japan Atomic Energy Agency; 3Department of Physics,
Tohoku University; 4Neutron Science Section, Materials and Life Science Division, J-PARC Center

1

40

Research and Development Highlights

Multiple-Probe Study of Highly Hydrogen Doped Fe-based
superconductor LaFeAsO1-xHx

2. Multiple probe measurement
Figure 1 (a) shows zero field μSR time spectra for x = 0.45 measured using GPS spectrometer at PSI. Spectra above 80 K show slow relaxation, which is attributed to a paramagnetic state,while spectra below 80 K exhibit an oscillation with
(a)

(b)

increased amplitude, indicating the development of
the magnetically ordered phase. The temperaturedependence of the magnetic volume fraction (MVF)
was measured using DΩ1 spectrometer installedat the MUSE D1 area of MLF J-PARC. As hydrogen content x decreases, the onset of the magnetictransition temperature TN and the MVF at the lowest
temperature decreases [2]. Summation of MVF andsuperconducting volume fraction determined fromsusceptibility measurement is almost unity, indicating that magnetic and superconducting phases coexist and phase-separates in 0.4 ≤ x ≤ 0.45, which
is a marked contrast to the underdoped region.
To investigate the magnetic structure, neutron powder diffraction in x = 0.45 and x = 0.51
samples was performed in NOVA and S-HRPD in
J-PARC MLF, respectively. Extra peaks indexed(1/2, 1/2, n)T,M (n = 0, 1, 2) were observed in the lowtemperature where the subscripts T, M and N referto the tetragonal cell, magnetic and nuclear peak,
respectively (Figure 1(b)). The temperature dependence of the Bragg peak intensity and the corresponding muon magnetic signal intensity (MVF x
precession frequency squared) is shown in Figure 1(c). Intensities of magnetic peaks develop below TN= 89(1) K, which is perfectly in line with the μSR result. Similar antiferromagnetic transition was also

Magnetism &Strongly Correlated Systems

1. Introduction
The recent development of the hydrogenation
technique in rare earth systems of Fe-based superconductors REFeAsO1−xHx (RE: rare earth) has
succeeded in surpassing the limitation of the doping
range available in fluorine doping [1]. In the case of
LaFeAsO1−xHx, the existence of a secondary superconducting dome (SC2) around 0.2 ≤ x ≤ 0.4 has
been revealed [1]. Moreover, the maximum Tc of~ 36 K in SC2 is higher than that of ~ 26 K in thefirst superconducting dome (SC1) around 0.05 ≤ x≤ 0.2, drawing broad attention regarding the difference in superconducting mechanism between SC1
and SC2. The relationship of SC2 with magnetism
would be of particular interest in comparison tothat of SC1. To investigate the origin of the two SC
domes, we have performed a multiple probe study
in the range 0.40 ≤ x ≤ 0.51 using muon spin rotation/relaxation (μSR), powder neutron diffraction(ND), and X-ray diffraction (XRD) [2].

(c)Figure 1.	(a) μSR time spectra of LaFeAsO1-xHx for x = 0.45. Spectra below 80 K exhibit fast relaxation with precession signal.
	(b) Neutron diffraction of x = 0.51 sample. At 10 K, there are additional Bragg peaks from magnetic order.
	(c) Temperature dependence of muon magnetic signal intensity (volume fraction x precession frequency squared) andneutron Bragg peak intensity.

Research and Development Highlights

41

observed below TN = 76 K for x = 0.45. The magnetic structure is displayed in the inset of Figure 1(c) and Figure 2. The spin arrangement is antiferromagnetic collinear structure, and the stacking ofneighboring plane along the c-axis is ferromagnetic.
The magnetic moment in x = 0.51 at 10 K is 1.21(1)μΒ, which is twice as large as that in x = 0 [3].
XRD of x = 0.51 performed at BL-8 in KEK-PF
reveals that (2, 2, 0)T reflection exhibits peak splitting
on cooling, whereas, that reflection of x = 0.45 exhibits simply slight broadening. In x = 0.51, (0, 0, L) reflection does not exhibit peak broadening, indicating
the occurrence of the tetragonal to orthorhombic (TO) structural transition. T-O transition temperatureµµMagnetism &Strongly Correlated Systems

Figure 2.	Crystal and magnetic phase diagram of LaFeAsO1-xHx.
Filled blue circles, green squares, triangles indicate antiferromagnetic transition temperature (TN)determined by μSR, structural transition temperature (Ts), and cT-axis upturn temperature (Ts’) determined by XRD, respectively. Insets show themagnetic structures of AF1 (left) and AF2 (right)
determined by neutron diffraction, and the structures of FeAs4 tetrahedron.

Ts ~ 95 K is determined from the temperature dependence of the lattice constant. Interestingly, cT
axis length shows an upturn below Ts. In x = 0.45,
although an apparent T-O transition does not exist,
the cT axis anomaly appears below Ts’ ~ 80 K as in
the case of x = 0.51, which may be attributed to theinsufficient coherence of the splitting of aT and bT in
the low-temperature phase. The crystal structure
below Ts in x = 0.51 is determined to be the orthorhombic Aem2 structure without inversion symmetry,
which is different from Cmme structure with inversion symmetry of x = 0 [3,4]. In the Cmme structure,
Fe atoms exhibit off-center deformation in the FeAs4
tetrahedron, as shown in the inset of Figure 2.
3. Phase Diagram and Discussion
The resultant temperature dependence of TN(determined by μSR), Ts and cT axis upturn temperature Ts’ are summarized in Figure 2. The newly discovered antiferromagnetic phase (AF2) precededby structural transition resembles the behavior of x
= 0 phase (AF1). The two-dome SC phase diagram
may be interpreted as the carrier doping startingfrom the left and right side of the parent compounds(x = 0 and x ~ 0.5), where the valley of Tc around x= 0.2 may be a crossover region or the over-dopingfrom both sides of the phase diagram.
References[1]	S. Iimura et al., Nat. Commun. 3 (2012) 943.
[2]	M. Hiraishi et al., Nat. Phys, 10, 300 (2014).
[3]	N. Qureshi et al., Phys. Rev. B 82, 184521(2010).
[4]	T. Nomura et al., Supercond. Sci. Technol. 21,
125028 (2008).

M. Hiraishi1, S. Iimura2, K. M. Kojima1,3, J. Yamaura4, H. Hiraka1, K. Ikeda1, P. Miao1,3, Y. Ishikawa1, S. Torii1, M. Miyazaki1,3,
I. Yamauchi1,3, A. Koda1,3, K. Ishii5, M. Yoshida5,6, J. Mizuki6, R. Kadono1,3, R. Kumai1,3, T. Kamiyama1,3, T. Otomo1,3,
Y. Murakami1,3, S. Matsuishi4, and H. Hosono2,4
1
Insitute of Materials Structure Science, KEK; 2Materials and Structures Laboratory, Tokyo Institute of Technology; 3Muon Science Section,
Materials and Life Science Division, J-PARC center; 4Materials Research Center for Element Strategy, Tokyo Institute of Technology;
5
SPring-8; 6School of Science and Technology, Kwansei Gakuin University

42

Research and Development Highlights

Long Periodic Chiral Helimagnetic Ordering in T1/3MS2(T = Transition Metal, M = Nb and Ta)

measurements show a variety of magnetic behaviors [6]; antiferromagnetism for Fe1/3NbS2, Co1/3NbS2,
Ni1/3NbS2, Co1/3TaS2 and Ni1/3TaS2, and ferromagnetism for Cr1/3NbS2, Mn1/3NbS2, Cr1/3TaS2, Mn1/3TaS2
and Fe1/3TaS2.
In our single crystalline magnetization data, someof the above-mentioned ferromagnetic T1/3MS2 compounds show the magnetization-cusp, indicating thechiral helimagnetic ordering and formation of a chiralmagnetic soliton lattice [7].
We performed super high resolution powder neutron diffraction experiments at BL08 (Super HRPD)
in the Materials and Life Science Experimental
Facility (MLF) of J-PARC. We obtained powder diffractograms of the ferromagnetic T1/3MS2. We succeeded in separating the nuclear and magnetic
satellite peaks in Cr1/3NbS2 and Cr1/3TaS2. Figure 1
shows the data around the (0,0,4) and the (1,0,3)
reflections. As indicated by the vertical arrows, themagnetic satellite peaks were observed at different
d values from the nuclear peaks, and were indexedwith the magnetic propagation vector kmag = (0,0,δ).
The periods of the incommensurate magnetic ordering were determined to be 600 angstroms for
Cr1/3NbS2 and 230 angstroms for Cr1/3TaS2. There
was no peak splitting in Mn1/3NbS2 and Fe1/3TaS2.
However, comparing the peak widths between paramagnetic and magnetic phase, we found apparent
increase of the peak width in the magnetic phaseof Mn1/3NbS2. If the increase is due to existence ofmagnetic satellite peaks, the period of the magnetic
ordering can be over 2000 angstroms.
With determined magnetic propagation vectors,
we performed magnetic structure analysis of theobtained diffraction data using Rietveld method.
While Fe1/3TaS2 forms ferromagnetic structure along
the c-axis, the magnetic structures of Cr1/3NbS2,
Cr1/3TaS2 Mn1/3NbS2 are well interpreted by helimagnetic structure in the a-b plane with very long period, which is unique to chiral helimagnetic ordering.

Research and Development Highlights

Magnetism &Strongly Correlated Systems

The concept of chirality, meaning left- or righthandedness, plays an essential role in symmetry
properties of nature at all length scales, from elementary particles to cosmic science. In materials
sciences, it is very important to understand the chirality in molecules, crystals and magnetic structures
both from theoretical and experimental viewpoints.
Recently, significant attention has been paid to therelationship between crystallographic chirality andthat of magnetic structure, because the sense of ahelical spin structure depends on the right- or lefthanded chiral crystallographic structure that allows
an asymmetric Dzyaloshinskii-Moriya (DM) interaction [1, 2]. Kishine et al. theoretically proposesthat the chiral helimagnetic compounds can exhibit
a new giant magnetoresistance effect due to theformation of a chiral magnetic soliton lattice [3, 4].
Under an applied field perpendicular to the helicalaxis in Cr1/3NbS2, the chiral magnetic soliton lattice
was observed by means of Lorentz microscopy [5].
However, there have been few experimental results due to the difficulty in synthesizing suitable materials to realize such research. In chiral helimagnetic compounds, the pitch angle, mainly determined by
the ratio of exchange interaction and DM interaction,
is usually very small. As a result, the helimagnetic
period can be hundreds of angstroms. Therefore,
sometimes the Q resolution of thermal neutron diffraction experiments is not high enough to separate
fundamental Bragg peaks and magnetic satellite
peaks. As a consequence, some compounds withchiral helimagnetic ordering may be easily misinterpreted as having ferromagnetic ordering. In thissense, high Q resolution is the key to detect the long
periodic helimagnetic satellite peaks.
T1/3MS2 (T = transition metal, M = Nb and Ta),intercalated system of 2H-MS2, has a chiral crystal structure with a chiral space group P6322. The
chiral space group allows DM vector parallel to the
crystallographic helical axis, and expects chiral helimagnetic ordering of the c-axis. Magnetization

43

5×10−1

6×10−1
4×10−110K
180K(1,0,3)(0,0,4)(b)

6×10−1

Intensity [a. u.]

Intensity [a. u.]

8×10−1

7×10−1

10K
160K(0,0,4)(a)(1,0,3)

1×100

4×10−1
3×10−1
2×10−1−1

2×10

1×10−1

Cr1/3NbS2
0
2.95

3

3.05

3.1

3.15

3.2

d [Å]

0
2.95

Cr1/3TaS2
3

3.05

3.1

3.15

3.2

d [Å]

Figure 1.	Powder diffraction profiles of the (0,0,4) and the (1,0,3) reflections in (a) Cr1/3NbS2 and (b) Cr1/3TaS2. The verticalarrows indicate magnetic satellite peaks.

Magnetism &Strongly Correlated Systems

References[1]	I. E. Dzyaloshinskii: J. Phys. Chem. Solids 4(1958) 241.
[2]	T. Moriya: Phys. Rev. 120 (1960) 91.
[3]	
J. Kishine, K. Inoue, and Y. Yoshida: Prog.
Theor. Phys. Suppl. 159 (2005) 82.
[4]	
J. Kishine, I. Proskurin, and A. Ovchinnikov:
Phys. Rev. Lett. 107 (2011) 017205.
[5]	Y. Togawa, T. Koyama, K. Takayanagi, S. Mori,

Y. Kousaka, J. Akimitsu, S. Nishihara, K. Inoue,
A. Ovchinnikov, and J. Kishine: Phys. Rev. Lett.
108 (2012) 107202.
[6]	S. S. P. Parkin and R. H. Friend, Phil. Mag. B
41 (1980) 65.
[7]	Y. Kousaka, Y. Nakao, J. Kishine, M. Akita, K.
Inoue, and J. Akimitsu, Nucl. Instr. Meth. Phys.
Res. A 600 (2009) 250.

Y. Kousaka1,2,3, T. Ogura1, J. Akimitsu1, K. Inoue2,3, J. Zhang4,5, P. Miao4,6, S. Torii4,7, and T. Kamiyama4,6,7
Department of Physics and Mathematics, Aoyama-Gakuin University; 2Graduate School of Science, Hiroshima University; 3Center for Chiral
Science, Hiroshima University; 4Institute of Materials Structure Science, KEK; 5IHEP, Chinese Academy of Science; 6Graduate University for
Advanced Studies (Sokendai); 7Neutron Science Section, Materials and Life Science Division, J-PARC center

1

44

Research and Development Highlights

Detailed Study of the Phase Diagram of Fe-Based
Superconductor Ba(Fe1-xCox)2As2

1200
1000

T * (?)

TN

Ort

Tc
SC

Co content, x

Figure 1. Phase diagram of Ba(Fe1-xCox)2As2.

T = 140.5 K

T = 141.0 K

T = 150.0 K

Magnetism &Strongly Correlated Systems

600
400
200

1000

Tet

T = 130.0 K

800

0
1200

TS

AFM/Ort

3. Results and Discussion
Fig. 2 shows the example profiles taken for
BaFe2As2. Their characteristics observed just below
TS ~ 147.5 K can be understood by considering thecoexistence of two Ort phases with different magnitudes of the orthorhombicity: the broad center peakconsists of two nearly Lorentzian-type ones with thesmaller orthorhombicity than that of the outer two, asshown in the fitted curves. The widths of the (h h l)O
Bragg reflections, the suffix o being the Ort notation,
were found not to split even below TS. In contrast, the(400)O / (040)O reflections, for example, exhibit significant T dependence in their width (FWHM) as shownin Figs. 3 and 4 even in the T region well above TS.

Intensity (a.u.)

Temperature (K)Ba(Fe1-xCox)2As2

2. Experiments
We used BL-08 Super-HRPD of J-PARC. To
avoid external stress from (1) surface effects, which
may exist in finely pulverized samples, and from(2) effects of grease or other glues used to fix asingle crystal sample to a holder, we used samples
consisting of assemblies of mm-size crystallites ofBa(Fe1-xCox)2As2. We also considered the effects ofimpurities doped to the system, and therefore usedsamples both with and without Co impurities.

Intensity (a.u.)

1. Introduction
There are two different proposals concerning thesuperconducting mechanism of Fe-based systems.
One of them considers the role of spin-fluctuation,
because the superconductivity appears near the
antiferromagnetic (AF) phase in the phase diagram(see Fig. 1 for Ba(Fe1-xCox)2As2, for example). The
other proposal considers the “orbital-fluctuation”
defined by the electron occupancies between the
3dyz and 3dzx orbitals, because of the common
existence of the tetragonal (Tet)-orthorhombic (Ort)structural transition found in various Fe-based systems at temperature TS slightly higher than the AF
transition temperature TN (see Fig. 1) [1].
In addition to the above two temperatures, TS andTN, another temperature T* (= TS + η, the η value being
not so clear but ~ 30 K at x ~ 0.02) has been added byobserving the breakdown of the four-fold symmetry(C4) of transport and other static quantities below T*(the so-called “nematic state”, TS < T < T* [2, 3]), andextensive arguments have been made on its possible
origin, because it is considered to be very informative
to identify the superconducting mechanism, namely,
to answer the question, “spins or orbitals?”.
To study this issue in detail, we have carried out
high-resolution neutron diffraction measurements,
and based on the details, we show what induces
the nematic state and approach the question about“spins or orbitals?”.

800
600
400
200
0
1.39

1.395

1.4

d (Å)

1.405

1.41

1.395

1.4

d (Å)

1.405

1.41

Figure 2.	
Example profiles obtained at (400)O/(040)O Braggreflections of BaFe2As2.

Research and Development Highlights

45

0.004

BaFe2As2

0.003

0.00250.002

0.0015Ba(Fe1-xCox)2As2
x=0
x = 0.02

0.0035400o / 040o

FWHM (Å)

FWHM (Å)

0.00350.003
0.0025
0.002

150

200

250

300

Temperature (K)350

0.001580 100 120 140 160 180 200 220 240 260

T (K)Magnetism &Strongly Correlated Systems

Figure 3.	
Width of the obtained (400)O/(040)O raw reflection
profiles against T.

Figure 4.	Temperature dependence of the width of the obtained (400)O/(040)O of x = 0 and 0.02.

Since T dependence becomes visible with decreasing T, say, at ~270 K, the T dependent behavior of
the width should begin at T higher than 270 K, because the value we observed includes the resolution
broadening. This indicates that the broadening issurely due to the existence of the Ort distortion. One
more thing we note here is that the FWHM exhibits
no anomaly in the T dependence at around T* (> TS).
The question is why the broadening appears. If
the Tet-Ort transition takes place homogeneously at
T*, we cannot expect the broadening on the Braggreflection above TS, because the dynamical fluctuation induces only the change of the Bragg intensity
through the Debye-Waller factor. However, in thenematic phase, there is evidence that various staticquantities exhibit the breakdown of the C4 symmetry there. Moreover, the softening magnitude of theelastic constant C66 reaches its maximum at TS [4],indicating that the almost second order transition
takes place at TS not T*.
It is interesting to show in Fig. 4 the T dependence of the profile widths of Ba(Fe1-xCox)2As2 with x= 0 and 0.02. We can see that the FWHM value increases with x in the high T-region. It is, we think, due
to the finite size Ort domains pinned by lattice defects
and Co impurities even at high T. It is consistent withthe theoretical arguments proposed by Inoue et al.
[5], which predicted the domain size of ~ 7 × 15 lattice spacing. The present picture is also consistent

not only with the experimental report by Luo et al. [6]that no anomaly has been observed in the precise
specific heat data at around T corresponding to T*,
but also with the fact that the largest softening of C66
is at x = 0, because as the volume fraction of the Ort
domains increases with x, the softening magnitude at
TS decreases. As T approaches TS, the Ort domains
around the defects prevail and the FWHM’s of the
Bragg profiles increase as shown in Figs. 3 and 4.
The imbalance of the Ort volumes with orthogonala- and b-axes is an origin of the observed anisotropyof various static physical properties.
Finally, from the rather wide T region of the widthchange found in Figs. 3 and 4, we think that the orbital
fluctuation would favor the origin of the nematic state,because the orbital-lattice coupling is larger than thatof the spin-lattice one, implying that the former may beclosely related to the origin of the superconductivity.
References[1]	H. Kontani and S. Onari, Phys. Rev. Lett. 104(2010) 157001.
[2]	J-H. Chu et al., Science 329 (2012) 824.
[3]	S. Kasahara et al., Nature 486 (2012) 382.
[4]	M. Yoshizawa et al., J. Phys. Soc. Jpn. 81(2012) 177001.
[5]	Y. Inoue, Y. Yamakawa and H. Kontani, Phys.
Rev. B 85 (2012) 224506-1.
[6]	X. Luo et al., arXiv:1407.6108 (2014).

K. Ikeuchi1, M. Sato1, S. Li2,3, M. Toyoda2,3, Y. Kobayashi2,3, M. Itoh2,3, P. Miao4, S. Torii4, Y. Ishikawa4, and T. Kamiyama4
1
Neutron R&D Division, CROSS-Tokai; 2Neutron Science Section, Materials and Life Science Division, J-PARC center; 3Insitute of Materials
Structure Science, KEK; 4Department of Physics, Nagoya University

46

Research and Development Highlights

Electrical Activity of Interstitial Hydrogen in BaTiO3
Simulated with Positive Muons

2. Muonium as a pseudo-isotope of hydrogen
The positive muon is a lepton with a charge +e
and a rest mass of 105.7 MeV/c2, which is about
1/9 of that of a proton. It is well established that apositive muon implanted in matter behaves as alight proton and creates a point defect analogous
to an interstitial hydrogen impurity. A muon-electron
bound state, called muonium, simulates the electronic state of interstitial hydrogen with high accuracy as shown in Fig. 1. Spectroscopic signals frommuonium can be sensitively detected thanks tomuon’s radioactive decay. Therefore, with positive

Figure 1.	A schematic illustration of muonium and hydrogenin vacuum (1s state). The Bohr radius of muonium is identical to that of hydrogen except for asmall correction (~ 0.5%) due to the difference of
reduced mass.

muons, one can imitate interstitial hydrogen impurities in BaTiO3 in dilute limit and selectively probe
their electrical activity.

Semiconductor

1. Introduction
Multilayer ceramic capacitors (MLCCs) are fundamental components of electronic circuits and indispensable for state-of-the-art electronic devices,such as smartphones. Since the performance of
MLCCs depends heavily on that of dielectric materials, the quality control of those is vitally important.
As typical MLCCs involve nickel (easily oxidizable
element) for internal electrodes, an annealing process to unify the dielectrics and internal electrodes
is performed in a reducing atmosphere containing hydrogen. On the other hand, this process cancause insulation degradation of dielectric layers
depending on the annealing conditions. Intensive
studies are under way to identify the origin of thedegradation.
In this work, we focused on the risk of unintentional incorporation of hydrogen into dielectric layers in the annealing process and studied its role inbarium titanate (BaTiO3), one of the most commonlyused dielectrics in MLCCs. Similarly to other band
insulators, the electronic properties of BaTiO3 canchange greatly upon the introduction of impurities.
However, it is very difficult to detect spectroscopic
signals from such trace amounts of hydrogen withconventional experimental techniques. To overcome this difficulty, we used positive muons insteadof hydrogen.

3.	Muon implantation experiments at the J-PARC
muon facility
A positive muon beam was irradiated to a single
crystalline sample of nominally undoped BaTiO3 at
the J-PARC muon facility and the local electronic
structure around implanted muons was investigatedby means of the muon spin rotation (µSR) technique. Details of the experiment were reported elsewhere [1].
Typical Fourier-transformed µSR spectra in atransverse field of 18.95 mT are shown in Fig. 2.
A symmetric broad feature was found below about
80 K together with a bare muon (Mu+) signal, assigned to paramagnetic muonium (Mu0). A hyperfine coupling constant of Mu0 was estimated to be~ 1 MHz from the line width, which is about 10-3
that in vacuum (4463 MHz). This suggests that anelectron cloud of Mu0 spreads over several tens ofunit cells in BaTiO3 as shown in Fig. 3, and thus
the electron binding energy is expected to be fairly
small.

Research and Development Highlights

47

Figure 2.	Fourier-transformed µSR spectra of BaTiO3 in atransverse field of 18.95 mT at 2.7 K (solid curve)and 225 K (broken curve). f0 = 2.569(1) MHz is a
Larmor frequency of Mu+.

Figure 4.	Ratios of muonium (Mu0) and ionized muonium(Mu+) signals as functions of temperature. Solid
curves represent the best fits to an ionization
model [3].

Semiconductor

minimum. The electrons released from the shallow
Mu0 can move freely around the crystal and lead toelectric conductivity, thus decreasing the insulating
performance of BaTiO3. Interstitial hydrogen impurities in BaTiO3 also seem to form a shallow donor
level in a similar way and cause insulation degradation at device operating temperatures.
The insights from this work can be applied to improve the performance of BaTiO3-based MLCCs by
reducing the risk of hydrogen incorporation in theirfabrication processes.
Figure 3.	
A schematic illustration of shallow muonium in
BaTiO3 and muonium in vacuum. The crystallographic illustration was produced by VESTA [2].

A Mu0-to-Mu+ conversion was observed with therise of temperature as shown in Fig. 4, interpreted as
an ionization process of Mu0. The ionization energy
was estimated to be ~ 10-2 eV based on an ionization model [3]. This is considerably smaller than theband gap of 3.2 eV and indicates that Mu0 forms ashallow donor level just below the conduction band

References[1]	T. U. Ito, W. Higemoto, T. D. Matsuda, A. Koda,
and K. Shimomura, Appl. Phys. Lett. 103,
042905 (2013).
[2]	K. Momma, and F. Izumi, J. Appl. Crystallogr.
44, 1272–1276 (2011).
[3]	S. F. J. Cox, J. L. Gavartin, J. S. Lord, S. P.
Cottrell, J. M. Gil, H. V. Alberto, J. Piroto Duarte,
R. C. Vilão, N. Ayres de Campos, D. J. Keeble, E.
A. Davis, M. Charlton, and D. P. van der Werf, J.
Phys.: Condens. Matter 18, 1079–1119 (2006).

T. U. Ito1,2, W. Higemoto1,2, A. Koda2,3, and K. Shimomura2,3
Advanced Science Research Center, JAEA; 2Muon Science Section, Materials and Life Science Division, J-PARC Center; 3Institute of Materials
Structure Science, KEK

1

48

Research and Development Highlights

Synthesis, Structure, and Conduction Mechanismof the Lithium Superionic Conductor Li10+δGe1+δP2-δS12

Figure 1.	Neutron Rietveld refinement pattern forLi10.35Ge1.35P1.65S12 at 300 K. Red: observed intensities; black: calculated intensities; blue: difference plot. The green markers indicate the positions of the diffraction lines.

Neutron diffraction data were obtained using
time-of-flight (TOF) diffractometers: SuperHRPD(BL08) [4] and iMATERIA (BL20) [5] at the Materialand Life science Facility (MLF) of the Japan Proton
Accelerator Research Complex (J-PARC). The diffraction data were collected for 12 h at several temperatures from 4.8 to 750 K. The structural parameters were refined using the Rietveld refinement
programs Z-Rietveld [6]. During the neutron data
analysis, the d region from 1.0 to 3.5 Å was used for
the Rietveld analysis. The Z-MEM program was employed during calculations based on the maximum
entropy method (MEM) [7]. Z-3D [8] was used to visualize the nuclear density map of the structure.

Battery Technology

1. Introduction
Among the various types of batteries currently
under consideration for future applications, the allsolid-state configuration has become a promising
candidate for high-energy and high-power-density
batteries [1, 2]. In order to develop all solid-state batteries, the key issue is the lithium superionic conductors, which could be used for the solid electrolyte.
Recently, a superionic conductor, Li10GeP2S12(LGPS), has been found to have high lithium ionic
conductivity of 10-2 S cm-1 at room temperature,
which is similar to the conductivity value of the liquid electrolyte used for lithium ion batteries [2, 3].
Although materials offering extremely high lithium
ionic conductivities have been developed, further
studies clarifying the conduction mechanism andincreasing the range of electrolyte materials arestill necessary to allow the practical applications ofthese electrolytes. LGPS is known to have a threedimensional framework structure composed of onedimensional chains formed by Ge(P)S4 tetrahedra
and LiS6 octahedra with edge sharing along the cdirection of the tetragonal structure [3]. These onedimensional chains are connected with each otherthrough PS4 octahedra by corner sharing.
Following the development of this LGPS-typeparent structure with extremely high ionic conductivity, it was recognized that similar solid solution
systems with different lithium contents might exhibit
even higher levels of ionic conduction. In addition,
cation and anion substitutions of the LGPS framework structure are also important means of achieving higher ionic conduction values. In the present
study, a solid solution with an LGPS-type structure
was produced based on a powder synthesis process that offers a practical means of fabricating solid
electrolytes. The composition and ionic conductivityof this new solid solution system, Li10+δGe1+δP2-δS12,
were subsequently examined and the conduction
mechanism within this material was studied using
neutron diffraction analysis.

2. Results and discussion
The LGPS solid solutions fabricated were basedon the Li3PS4 – Li4GeS4 pseudo-binary system, andcompositions similar to the parent LGPS (Li10GeP2S12)
phase were synthesized according to the compositional formula Li10+δGe1+δP2-δS12. Structural analysis
was carried out based on a previously reported model incorporating three lithium sites (Li1 at 16h: x, y, z;
Li2 at 4d: 1, 1/2, z, Li3 at 8f: x, x, 0), together with an
Li4 site (Li4 at 4c: 0, 0, z) proposed as the result ofmolecular dynamics simulations [9]. Lithium ion distribution was visualized using the MEM analysis inconjunction with the neutron diffraction data obtainedfor Li10.05Ge1.05P1.95S12 (δ = 0.05) at 100 and 750 K.

Research and Development Highlights

49

Figure 2.	Atomic distributions in the Li10.05Ge1.05P1.95S12 (δ = 0.05) unit cell at 100 K (a) and 750 K (b). The probabilityof an atom being present is indicated only for the negative scattering powers, which corresponds to thelithium ion distribution.

Battery Technology

Figure 2 shows the atomic distribution in the unit
cell, in which the probability of an atom being present
is represented only for the negative scattering powers,
which corresponds to the lithium ion distribution. At
100 K, the Li1, Li1, and Li3 sites are connected along
the c-axis, while the other lithium sites (the Li2 and Li4
sites) are isolated from each other. The one-dimensional conduction pathway represents the primarymeans of lithium ion conduction at 100 K and this conduction pathway becomes more evident at 750 K. In
addition, continuous lithium distribution between theLi1 and Li4 sites is now observed. These results demonstrate that the lithium conduction takes on a threedimensional character, as opposed to the one-dimensional at higher temperatures. The LGPS structure isevidently well-suited to a three-dimensional conduction. Even though the one-dimensional conduction isdominant at lower temperatures, the pathway over theab plane becomes evident at high temperatures.

References[1]	X. Xu et al., Chem. Mater. 23 (2011) 3798.
[2]	Y. Kato et al., Electrochemistry 80 (2012) 749.
[3]	N. Kamaya et al., Nat. Mater. 10 (2011) 682.
[4]	S. Torii et al., J. Phys. Soc. Jap. 80 (2011)
SB020.
[5]	T. Ishigaki et al., Nucl. Inst. Meth. Phys. Res. A
600 (2009) 189.
[6]	R. Oishi et al., Nucl. Inst. Meth. Phys. Res. A
600 (2009) 94.
[7]	J. Zhang et al., Z-MEM, Textbook of Z-Code
Powder diffraction data analysis school, Tokyo,
Japan, Mar 25-26, 2014.
[8]	Y. Ishikawa et al., Z-3D, Textbook of Z-Code
Powder diffraction data analysis school, Tokyo,
Japan, Mar 25-26, 2014.
[9]	S. Adams et al., J. Mater. Chem. 22 (2012)
7687.

O. Kwon1, M. Hirayama1, K. Suzuki1, Y. Kato2, T. Saito2, M. Yonemura3,4, T. Kamiyama3,4, and R. Kanno1
1
Department of Electronic Chemistry, Tokyo Institute of Technology; 2Battery Research Division, Higashifuji Technical Center, Toyota Motor
Corporation; 3Neutron Science Section, Materials and Life Science Division, J-PARC center; 4Insitute of Materials Structure Science, KEK

50

Research and Development Highlights

Development on Non-Destructive Elemental Analysis
for Extraterrestrial Materials using a Muon Beamof rocky samples by changing the momentum of themuon beam. Here, we report on the first trial of thedepth profile analyses of a rock-sample simulant
and carbonaceous meteorites [7]2. Experiment 1 ~ depth profile analysis ~At first, we tried the depth profile analysis of the
four-layered sample that consists of SiO2, C (graphite), BN (boron nitride) and SiO2 using the D2 beamline at J-PARC MUSE, each with thickness of 1.5,
1.0, 1.3 and 1.5 mm. The negative muon beam
was collimated to approximately 27 mm in diameterand focus on the 50 mm *75 mm *5.3 mm sample
that was oriented at 45 degree to the beam. Bychanging the Muon’s momentum from 37.5 MeV/c
to 57.5 MeV/c, the generated high energy muonic
X-rays were measured by two Ge detectors (onewas planar type (LEPS) and the other was coaxial
type (Loax)). Figure 1 shows the X-ray spectra obtained by LEPS. Our preliminary result successfully
demonstrates that the muon beam analysis has a

Microanalysis &Non-destructive analysis

1. Introduction
In 1971, Rosen [1] noted the great availability ofmuon beam analysis and proposed its applicationin the chemical analysis of tissues, as muon beam
analysis would cause less damage to the host organism than neutron activation analyses. Muonic
atom spectroscopy has been developed over the
past four decades [2-4] as a non-destructive analytical method; however, for a real application, one
had to wait for an intense muon source. The intense
pulsed muon source, J-PARC MUSE (Japan Proton
Accelerator Research Complex, MUon Science
Establishment), was constructed and succeeded inproviding a decay muon rate of 106 s-1 for a momentum of 60 MeV/c in November 2009, which is themost intense pulsed muon beam in the world [5, 6].
The stopping distances of both negative muons(~ tens of MeV/c) and muonic X-rays (more thanseveral tens keV) are in the ranges of millimeters,
which could potentially enable us to obtain the 3-D
elemental map from the near surface to the interior

Figure 1.	Muonic X-ray intensities are shown in arbitrary units with offset to compare the spectra
obtained with different muon momenta (37.5-57.5 Mev/c).

Research and Development Highlights

51

potential to map non-destructively 3-D elemental
distributions of light elements such as B, N, C, andO. The depth resolution is currently estimated tohave a 10% uncertainty against the mean penetration depth of the muons.
3.	Experiment 2 ~ elemental analysis of meteorite sample ~Next, we carried out X-ray fluorescence spectroscopy for carbonaceous chondrites, Murchison
and Allende. The negative muon beam, collimatedto approximately 40 mm in diameter, irradiated to a
~ 5-mm-thick Murchison disk with the exposed surface area of ~ 50 mm × ~ 100 mm. Aluminium foil
was used to hang the sample inside the chamber.
The exposure time was approximately 13 hours,
and the momentum of the incident muon beam wasset at 16 MeV/c, corresponding to the penetration
depth of ~ 70 μm. For Allende meteorite analysis,

the muon beam was collimated to approximately
27 mm in diameter at the sample surface of 50 mm
× 75 mm. The sample was also hung with lessamounts of Al holder than for the Murchison meteorite to reduce the background signal of Al. The exposure time was approximately 10 hours, and the incident muon momentum was set at 34 MeV/c (withpenetration depth of ~ 1 mm). As shown in Figure 2,
significant counts of fluorescent X-rays of Mg, C, Si,
Fe, Ca, and S from Murchison and those of Mg, Si,
Fe, K, and Ca from Allende were detected. On theother hand, those of K from Murchison and C andS from Allende were not detected. This indicatesthat the detection limit of muonic fluorescent X-ray
at the current analytical condition is about 1 weightpercent in concentration. It should be noted that thesignal of Al is background signal from a vacuum
chamber and/or a sample holder.

Microanalysis &Non-destructive analysis
Figure 2.	Muonic X-ray energy spectra from carbonaceous chondrites: Allende (red) and
Murchison (blue) meteorites.

52

Research and Development Highlights

4.	Experiment 3 ~ “see-through” analysis of
Murchison in glass tube ~Finally, we tried the measurement of Murchison
meteorite sealed in a glass tube as a simulant of
Hayabusa 2 samples collected from a C-type asteroid. Powdered Murchison meteorite weighing
610 mg was placed in a 50-mm-long SiO2 glass
tube, with inner and outer diameters of 4 and 6 mm,
respectively. The muon beam collimated to approximately 25 mm in diameter, and the apparent crosssection of the sample was 4 mm × 25 mm. After
exposure to the muon beam with momentum of
37 MeV/c for approximately 24 hours, clear signalsof Mg and marginally resolved signals of Fe weredetected through the 1-mm thick glass wall (Fig. 3).
Although O and Si are the major elements of rocksamples, muonic X-rays of O and Si were emitted
from the SiO2 glass tube as well, which cannot be
distinguished from the sample signals. Althoughfurther developments in analytical techniques are
required, such as detector setting and collimationof the incident muon beam, our first attempt for the
non-destructive elemental analysis of an extraterrestrial sample inside a glass tube succeeded withthe detection of Mg and Fe.

References[1] L. Rosen, Science 173, 490–497 (1971).
[2]	H. Daniel, Nucl. Instrum. Methods Phys. Res.,
B 3, 65–70 (1984).
[3]	M. K. Kubo et al., J. Radioanal. Nucl. Chem.
278, 777–781 (2008).
[4]	K. Ninomiya et al., Bull. Chem. Soc. Jpn. 85,

Microanalysis &Non-destructive analysis

Figure 3.	Muonic X-ray spectra from the powdered Murchison meteorite in a SiO2
glass tube.

228–230 (2012).
[5] D. Cyranoski, Nature 456, 426–427 (2008).
[6]	Y. Miyake et al., Nucl. Instrum. Methods Phys.
Res., A 600, 22–24 (2009).
[7]	K. Terada et al. Nature Scientific Reports 4,5072 (2014) DOI: 0.1038/srep050.

K. Terada1, K. Ninomiya1, T. Osawa2, S. Tachibana3, Y. Miyake4,5, M. K. Kubo6, N. Kawamura4,5, W. Higemoto7,
A. Tsuchiyama8, M. Ebihara9, and M. Uesugi101
Graduate School of Science, Osaka University; 2Quantum Beam Science Center, JAEA; 3Graduate School of Science, Hokkaido University;
4
Muon Science Section, Materials and Life Science Division, J-PARC Center; 5Muon Science Laboratory, IMSS, High Energy Accelerator
Research Organization; 6Graduate School of Science, International Christian University; 7Advanced Science Research Center, JAEA;
8
Graduate School of Science, Kyoto University; 9Graduate School of Science and Engineering, Tokyo Metropolitan University; 10JAXA Space
Exploration Center, Japan Aerospace Exploration Agency

Research and Development Highlights

53

Superconducting Nanowire Neutron Detector

1. Introduction
Pulsed neutron sources such as J-PARC [1]have made an important impact in various branchesof sciences and technologies, i.e., material analyses aiming at identifying the location of light atoms(hydrogen, carbon, and others) by means of neutron radiography. For example, one can observe
the dynamics of carbons and water molecules inoperating fuel cells and engines [2]. Spatial resolution remains on the level of several tens mm even in
high-end neutron detectors [3].
We proposed a current-biased kinetic inductance detector (CB-KID) made of Nb nanowire. We
intend to build a Nb CB-KIDs with the 10B conversion layer [4]. We report the results of successful
neutron detection using a CB-KID detector with the10
B converter at J-PARC.

Detector & Device

2. Current-biased kinetic inductance detector
The kinetic inductance Lk of a superconductor isexpressed as Lk = msl/nsqs2S, where ms is the massof the Cooper pair, ns is the density of the Cooper
pairs, qs is the electric charge for the Cooper pairs,l is the nanowire length in total, and S is the crosssection area. A Nb-based kinetic inductance detector is fed by the DC bias current Ib through a bias
resistor. The voltage V across the detector is expressed by V = IbdLk/dt + LmdIb/dt ≃ IbdLk/dt, where
the magnetic inductance Lm is supposed to be independent of time. This utilizes the method for sensing
the dynamic nature of quasiparticle excitations andhence provides rapid response.
The nuclear reaction of 10B with neutrons releases a huge amount of nuclear energy of 2.31 MeV
or 2.79 MeV into restricted regime. In Fig. 1, we
schematically show the method of how to identify
the neutron arrival onto the detector. In the neutron
reaction 10B(n,4He)7Li, the two charged particles 4He
and 7Li are simultaneously emitted in the opposite
directions. Nuclear reaction energy would be used
to break some Cooper pairs in the superconducting

54

Research and Development Highlights

Nb nanowire and to cause a change in kinetic inductance in some portion of the nanowire.
A microwave kinetic inductance detector (MKID)
has been remarkably successful because the frequency domain multiplexing can be achieved by asingle stripline with many resonators [5]. It is also
beneficial for MKIDs not to have DC bias current
to reduce the Joule heating. However, the speed of
the MKID system is not so fast, and remains on theorder of ms. In the resonance circuit of the LC tank,there is a continuous energy exchange between the
L component and the C component, which would
prolong the overall response time of the detector
while the quasiparticle dynamics itself is very fast,
presumably on the order of ps. The Nb nanowire
has been successfully used as a superconducting
detector for various purposes.
Our CB-KID absolutely requires installing DC bias
current leads, in which heat dissipation distributes

Figure 1.	
A Nb nanowire detector with the 10B converter. Achange in kinetic inductance is detected by readout circuits.

along the current leads. Usually, the multiplexingof the current bias leads to enhancement in Joule
heating. We will explain how a series connection of
CB-KIDs in the superconducting state works at 4 K.
Even if we have many nanowires, we only need twolines which give the pathway for the incoming andoutgoing currents between room temperature and4 K. The request for exciting many CB-KIDs in viewof wiring is not a heavy burden in terms of cryogenics design because there are only two leads.
3. Neutron irradiation to CB-KID
We carried out a neutron irradiation experiments
to the Nb-based CB-KID with 10B converter at the
MLF (Materials and Life Science Experimental
Facility), J-PARC. We used beam line NOBORU(BL10) [1]. The operating power of J-PARC was
300 kW, and this gave us 3 × 107 neutrons/s/pulse
at BL10. The MLF pulse appears every 40 ms. We
used a bismuth crystal filter of 50 mm thickness to
reduce the burst gamma rays. As a result, the neutron intensity becomes 1.5 × 107 neutrons/s/pulse at
the Nb-based CB-KID detector with 10B converter.
The CB-KID consisting of superconducting Nb
can be used as a neutron detector by overlaying a
10
B converter layer. The thickness of the Nb CB-KID
is chosen as 40 nm and the line width is chosen as
1 mm on a single chip (22 mm × 22 mm silicon). At
the center of the chip, the effective area (8 mm ×8 mm) is covered with a 200 nm thick 10B converter
layer, deposited by an electron beam evaporator
under ultra-high-vacuum.
The Nb-based CB-KID detector was installed in a
4-K Gifford-McMahon (GM) refrigerator so as to coolthe detector down to 4 K. We used a Nb wire of 1 mm
width detector by feeding 100 mA as a bias current.
In Fig. 2, we show that a signal from the CB-KID detector is of width on the order of ns. A signal was amplified by a differential low noise amplifier (NF SA430F5, bandwidth 120 MHz), and was directly observed by a 2.5-GHz sampling digital oscilloscope.
We tried to observe the signal of the CB-KID
when the neutron shutter of BL10 was closed. We
were not able to observe any signal from the detector. On the other hand, a clear signal appeared,
as shown in Fig. 2, when the neutron shutter was
opened. This ensures that our CB-KID can detect
neutron from the pulsed neutron source at J-PARC
for the first time.
We succeeded in measuring the neutron flux
from pulsed neutrons at BL10 of J-PARC as a function of time. As shown in Fig. 3, a histogram of averaged neutron in 0.1 ms mesh is in good agreement with that of the simulation. The vertical scale
is divided by arrival time t to compensate a velocitydependent cross section between neutron and 10B.
This is convincing evidence that our detector successfully detected pulsed neutrons from J-PARC.

40

V [mV]

30

Detector & Device

Shutter open
1 µm meander line
T = 3.4 K
Ib = 100 µA
J = 0.25 MA/cm2

20
10
0
–10
–400

–200

0

200

400

Time [ns]Figure 2.	
Signal from CB-KID when the shutter is opened. The temperature is 4.05 K, the bias current is
100 mA, and the Nb linewidth is 1 mm.

Research and Development Highlights

55

40

∆t = 0.1 ms
T = 3.4 K
Ib = 100 µA
1 µm × 512 mm

Number of events/t [1/ms]

simulation
30

20

10

0

0

5

10

15

20

25

30

35

40

t [ms]
Figure 3.	
Averaged neutron flux as a function of time. The blue dash line shows the simulation result at BL10.

4. Conclusions
We demonstrated the sound operation of thenovel CB-KID made of Nb nanowires operating at
4 K. The operating speed of CB-KID is much fasterthan an MKID [5]. The Nb-based CB-KID with 10B
conversion layer can work as a neutron detector.
The devices were fabricated in CRAVITY facilities at AIST. This work is partially supported
by Grant-in-Aid for Scientific Research (S) (No.
23226019) and Grant-in-Aid for Young Scientists(B) (No. 26820130) from JSPS.

References[1]	F. Maekawa et al., Nucl. Instrum. Meth. A, 620(2010) 159.
[2]	I. Manke et al., Appl. Phys. Lett., 90 (2007)
184101.
[3]	S. Tremsin et al., Nucl. Instrum. Meth. A 652(2011) 400.
[4]	T. Ishida et al., J Low Temp. Phys. 716 (2014)216.
[5]	J. Zmuidzinas, “Superconducting Microresonators:
Physics and Applications”, Annual Review ofCondensed Matter Physics, Vol. 3: 169-214,
March 2012.

Detector & Device

S. Miyajima1,2, H. Shishido1,2, Y. Narukami1, N. Yoshioka1, A. Fujimaki3, M. Hidaka4, K. Oikawa5, M. Harada5, T. Oku5,
M. Arai5, and T. Ishida1,2
1
Department of Physics and Electronics; 2Insitute for Nanofabrication Research, Osaka Prefecture University; 3Nagoya University; 4Advanced
Industrial Science and Technology; 5Materials and Life Science Division, J-PARC Center

56

Research and Development Highlights

Neutron Source

Progress of the Neutron Source Section

1. Mercury target system
In order to operate the pulsed spallation neutron
source of J-PARC steadily under the rated proton
beam of 1 MW, the most critical issue is to mitigatepressure waves generated in the mercury target by
injecting intense proton beam, because it induces cavitation damage on the target vessel, which
shortens its lifetime. To overcome this issue, we developed a technique to inject gas micro-bubbles into
mercury. In 2012, for the first time in the world, we
started supplying helium gas micro-bubbles in therunning mercury circulation loop and confirmed thatthe vibration velocity on the target vessel initiatedby the pressure waves was definitely decreased.
However, the flow rate of helium gas did not reachthe rated value because mercury was unexpectedly intruded from a vent line to a helium supply line
through a surge tank.
Therefore, the most important task in 2013 wasto recover the flow rate of gas-microbubbles in the
mercury circulation system. During the maintenanceperiod, we removed the mercury from the heliumgas supply line by hands-on work and installed agas-liquid separator as a counter measure. We also
replaced the helium gas supply device with a newone with remote handling tools such as a masterslave manipulator and an in-cell crane.
As a result, the flow rate of gas micro-bubbles
in the mercury was successfully increased from
2.5 l/min to 7.5 l/min suppressing the vibration velocity of the target vessel by 1/3 to 1/4.
2. 3 GeV proton beam transport facility
Flattening the proton beam profile is another effective technique to suppress the pressure wave
generated in the mercury target, because theamount of cavitation damage is proportional to the
4th power of the beam power. Since the current proton beam profile has a Gaussian distribution, we
have installed two octupole magnets to suppress
the beam profile upstream of the muon production

58

Neutron Source

target in the 3 GeV proton beam transport line.
We investigated the performance of the ocutuplole
magnets during the accelerator study period in
February, 2014, and obtained a promising result,confirming that the peak of the proton beam profile
has been reduced by about 40%.
At the end of the 3 GeV proton beam transport
line, a proton beam window has been installed tocreate a boundary between the high vacuum environment in the transport line and the helium environment in the helium vessel, in which the targetmoderator-reflector system is placed. During themaintenance period, the proton beam window was
replaced for the first time. It was attached at the bottom of a 4-meter tall steel shielding plug and highly
activated. It was lifted up into a big shielding caskwith a remote handling gripper in it on the top of theneutron source station, and then moved to a storage area on the basement floor.
3. Cryogenic hydrogen circulation system
We replaced the accumulator of the cryogenic
super-critical hydrogen circulation loop during themaintenance period. It has a bellows structure enclosing helium to make its volume variable up to
6.85 L so that it could control the pressure rise in
the hydrogen loop induced by nuclear heating of
3.8 kW at the moderators when the 1-MW pulsed
proton beam injects or stops.
The new accumulator has a diameter of 300 mm
and unrestricted length of 85 mm, the same specifications as for the current accumulator. As the bellows consists of 5 blocks of welding bellows with
17 units in each of them, the plate thickness wasincreased from 0.4 mm to 0.8 mm in order to withstand a high pressure of 2.0 MPa. We inspected
carefully the welding process and improved it
through manufacturing a prototype of one blockof welding bellows. Consequently, we successfully
manufactured bellows that can expand and contractsmoothly without hysteresis.

We also confirmed through actual operation with
300 kW proton beam that the pressure rise in the
cryogenic super-critical hydrogen loop was mitigated at 20 kPa and it could reach 60 kPa for the 1 MW
operation, which satisfied the design requirement.
4. Updates of the neutron shutter system
The neutron shutter system of J-PARC is driven
by an electric servo motor. Since the operational
beam power increased up to 200 kW in 2011, a
failure indicating servo motor error occurred randomly several times. We found that it was caused
by a single event effect at the semi-conductor partof the servo amplifier by neutrons produced at
the target-moderator-reflector system. Therefore,
all servo drives of the shutter system were replaced to the robust type, which does not include
semi-conductors.
Further, in accordance of the construction of
new instrument of imaging BL22, a shutter gate withthree neutron extraction holes was newly manufactured and installed at the neutron source station.

5. Fabrication of spare components
In 2012, we started fabrication of a spare target
vessel which has a double-wall structure with a narrow width of 2 mm at the beam window portion in viewof extended lifetime of the target vessel. This designconcept has been already adopted at the Spallation
Neutron Source (SNS) of Oak Ridge National laboratory, showing that the pitting damage did not affectthe outer wall, while the inner plate suffered damage in the form of penetration holes through the operating period of 2500 MWh (about half a year with
1 MW proton beam). In 2013, the spare target wascompleted and delivered to MLF. This type of target
vessel would be in use from the latter half of 2014.
We have also started fabrication of a sparemoderator (coupled moderator) and a reflector. It isestimated that manufacturing period will take three
years. Calls for bids on the second decoupled andpoisoned moderator will be started in 2014 and2015, respectively. After all, the replacement of themoderator-reflector system is scheduled for 2019,
which is based on the estimation that the lifetime ofa moderator comes after a 6 MWy-irradiation.

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

Neutron Source

59

Status of Proton Beam Commissioning of MLF

1. Beam commissioning
Due to the incident, which happened at the hadron hall of J-PARC, the user beam operation of MLF
was canceled from the end of May to the end of July
2013. To avoid further incidents caused by the highpower proton beam, we carefully reviewed our instruments and concluded that we can rely on themto prevent incidents. In the summer of 2013, a super conducting LINAC was installed to increase thebeam energy from 181 MeV to 400 MeV. Due to thelower acceleration at the Rapid Cycling Synchrotron(RCS), which accelerates the proton beam to
3 GeV, the transverse emittance of the beam wasincreased at the exit of RCS. We assumed that thebeam loss might increase along the beam transport line. The beam loss was, however, similar tothe previous one. At the downstream near the muon
production target, called M1, we observed a minor
increase in the activation, mainly due to the radiation produced at the target.
Below we describe two subjects, which are topics of the beam commissioning: 1) The proton beam
window was replaced; the window is a physicalboundary between the high vacuum region at theaccelerator and the helium area around the neutron
target station. 2) To mitigate the damage at the mercury target vessel, octupole magnets were installedat the beam transport to reduce the peak current
density at the target.
2. Replacement of proton beam window
In order to determine the lifetime of the proton
beam window (PBW), made of aluminum alloy(Al5083), we watched the status of the PBW fromthe mercury target side. By placing a high zoom
WEB camera and LED light, the surface of the PBWon the helium vessels side was clearly observed asshown in Fig. 1. At the center, a clear beam footprint
was found. Some strange spots were found aroundthe corner of the PBW. If those spots were causedby refraction or shadow, those spots could have60

Neutron Source

Figure 1.	Surface of the 1st PBW observed by high zoom
WEB camera in October 2012.

been eliminated by changing the camera position.
However, regardless of the camera position, spots
were still found around the corner of the PBW, so we
decided to replace the PBW in the summer of 2013.
This was the first PBW replacement ever. Since
the cooling water for the PBW had high activation,such as 5000 Bq/cc, the work had to be done carefully, especially when detaching the coupler for thewater channel. To avoid contamination of radioactivity, a special house with local ventilation system
was temporally built on the PBW. Since water could
be evacuated completely and not a single drop ofwater remained in the channel, the decoupling work
could be performed smoothly. Despite a few minor
incidents during the replacement, such as breaking
of a driven chain for the hatch in the cask, the replacement work was completed successfully. The
seal performance of the new PBW was better thanthat of the first PBW.
The surface status of the first PBW after it wasplaced at the hot cell is shown in Fig. 2. Around thecorner, we found many pitting holes. On the other
hand, pitting holes could not be found at the center of the window. At the first mercury target vessel,
the nickel mirror, which was placed for measurement of the vessel’s vibration by the Laser Doppler
Bibrometer, was completely corroded. The pitting

Figure 2.	Surface of the 1st PBW at the helium vessel sideobserved at the hot cell.

Figure 3. Octupole magnet installed at the beam transport.

holes were probably caused by reaction with theacid produced by the radiolysis of the impurity gas
in the helium vessel. We concluded that the lifetimeof the first PBW was determined by the corrosion
due to acid in the helium vessel. To confirm the seal
performance of the helium vessel, helium leak examination was performed and a small amount ofleaking gas was detected. Due to radiation damage, the proton beam window has a life of about
3 years [1]. The examination of the surface status
was important to estimate the lifetime. By observing
the surface of the second PBW in the summer of2014, we will determine its lifetime.

magnet, two additional steering magnets were installed as well. For beam centering at the octupole,beam position monitors were installed at each octupole magnet. In the end of October 2013, the installation of the octupole magnets had finished, as
shown in Fig. 3.
In February 2014, we performed beam tests withthe octupole magnet. It was found that the beam
shape complied with the design calculations. By excitation of the octupole magnet, the beam halo wasconverged at the target center. It was also foundthat the beam heat load in the vicinity of the target
decreased.
To use safely the muon production target, which
was a fixed target made of carbon graphite, until thesummer of 2014, care of the beam treatment on themuon production target was required. To mitigate
the damage at the muon target, the beam position
was periodically shifted by creating a bump orbit.
The octupole magnet cannot be utilized for the normal user beam operation with the bump orbit at themuon target because it makes current density peaks
at the edge of the mercury target. After replacing theold one with a new rotating muon production target
planned for September 2014, the octupole magnet
can be utilized for user beam operations.

3. Installation of octupole magnet
In FY2012, octupole magnets were fabricatedfor beam flattering to decrease the peak current
density at the mercury target. The installation of theoctupole magnets began in September 2013 at thebeam transport. For beam flattering in horizontal
and vertical direction, two sets of octupole magnets
are required. An octupole magnet for the horizontal
direction was installed at the ceiling of tunnel M1
with open shielding, placed at about 5 m upstreamof the muon production target. That was the firstsuch trial after the facility was built. Due to the greatearthquake, the gap of shielding at the ceiling was
unusually narrow so that the moving of the shielding was difficult. For beam centering at the octupole

Reference[1]	S. Meigo et al., Nucl. Matter 450 141-146 (2014).

S. Meigo1, M. Ooi1, A. Akutsu1, T. Kawasahi1, M. Nishikawa1, K. Ikezaki1, and H. Fujimori2,3
Neutron Source Section, Materials and Life Science Division, J-PARC center; 2Muon Science Section, Materials and Life Science Division,
J-PARC center; 3Institute of Materials Structure Science, KEK

1Neutron Source

61Improvement of Pressure Wave Mitigation Functionin Mercury Target System62

1. Introduction
In order to mitigate pressure wave which causes
pitting damage to the inner surface of the mercury
vessel, micro bubbles of helium gas are injected
into the mercury using the gas supply system installed on the target trolley. Helium gas used as thecover gas in the surge tank is compressed in thegas supply system and supplied to the bubbler inthe target vessel. Helium gas accumulated on theupper surface of the mercury vessel flows into thesurge tank through the vent line. When the operation of the gas supply system started in FY2012,
we noticed that mercury unexpectedly intruded
into the helium supply piping and the helium supply
into the mercury circulation system was disturbed.
The pressure difference in the vent line squirted
mercury into the helium supply piping which was
positioned at the opposite side of the vent line outlet at the top of the surge tank as shown in Fig. 1.
In order to prevent the mercury intrusion into thehelium gas piping, the valve on the vent line wasclosed, but the accumulated helium gas at the outlet of the mercury target clogged the main mercury
pipe and the mercury flow rate decreased by 14%.
Because the helium gas going back to the surge
tank from the target vessel decreased, the heliumgas supply to the bubbler also decreased, which
led to the inadequate effect of the pressure wave
mitigation.

In order to recover the pressure wave mitigation
function in the mercury target system, the mercury in the helium gas piping was discharged by thehands-on work in the hot cell and a gas-liquid separator was installed by remote-handling.
Also, the pressure gauges in the mercury circulation system malfunctioned due to radiation damage and these pressure gauges were exchanged.
In this chapter we will show the details of thesechallenging maintenance works.

Figure 1.	A schematic drawing of the mercury inflow in thehelium gas line of the mercury target system.

Figure 2.	A schematic drawing of the vacuum system for thedischarge of the mercury in the helium gas piping
and photograph of the discharge work using thevacuum system in a hot cell.

Neutron Source

2.	Discharge of mercury in Helium gas line andinstallation of gas-liquid separator in vent line
The discharge work of mercury in the heliumgas line was performed with exchange work of thegas supply system to take away the mercury whichblocked helium gas flow. Two methods for mercury
discharge without the release of tritium in the helium gas line were applied. The first method involveda mercury collection pot with gas-liquid separate
function set in the helium gas line and the mercury
between the mercury target vessel and the gas supply system was discharged by pressurization (gasflow rate: ca. 10 m3/h) from the mercury target vessel side. Mercury of ca. 150 cm3 was collected. In
the second method, a vacuum system as shown in
Fig. 2 was prepared and a part of the helium gas
line was cut paying the closest attention not to release mercury vapor ant tritium. The mercury was4. Effect of the recovery in the helium gas line
Time histories of the helium flow rate of the
bubbling and the vibration velocity of the mercury
vessel before and after the maintenance works
are shown in Fig. 4. The helium flow rate was lessthan 0.1 m3/h before the maintenance work, but it
increased by 4 times after the maintenance work.
Looking at Fig. 5, the vibration of the mercury target
vessel could be reduced to about 1/3.
(a) 0.5

Helium flow rate, m3/h

3. Exchange of pressure gauges
The radiation resistance of these pressure gauges was improved to prolong the lifetime by increasing the shielding performance of the shielding box
including the pressure gauges. 7 pressure gauges
in the mercury circulation system were exchanged
by remote handling in about 2 weeks. In order tominimize the release of radioactive gas including
tritium gas, the mercury circulation system wasevacuated by the off gas process system to makethe air flow from the atmosphere to inside the mercury circulation system. The pressure gage nozzles
which were open to atmosphere were closed byrubber plugs when the pressure gauges were removed. It was confirmed that Osmium (Os185) adhered to the wetted surface of the flange as shownin Fig. 3 and the maximum dose of the flange was
150 mSv/h.

Figure 3.	Photograph of the flange of the pressure gauge
after removing the pressure gauge.

(b)
Normalized velocity, V/Vw/o bubble

sucked up from the end of the cut helium gas line.
The vacuum system was a closed loop consisting of a nozzle, a collection pot with the gas-liquid
separate function and a vacuum pump. It was possible to discharge about 1000 cm3 of mercury, whichmatched projected amount.
Since there was a possibility that the mercury
could come again into the gas supply system, agas-liquid separator was installed in the vent line.
The mercury collected by the gas-liquid separator isreturned to the mercury circulation loop and the helium gas goes back to the surge tank. Thanks to thegas-liquid separator, the operation using the ventline is possible and the flow rate of helium gas forthe bubble injection becomes 4 times higher thanthat before the maintenance.
The gas supply system was replaced, because
mercury accumulation was confirmed in it. The new
one has another gas-liquid separator to avoid mercury accumulation into the system due to the remaining mercury which could not be removed during the above-mentioned maintenance works.
These maintenance works were carried out
in about three months and required about 250
man-days.

0.4

Before
Aer

0.3
0.2
0.1
0
11/1 1/1
2013

1

3/1

5/1

2/1
2014

4/1

6/1

Before
Aer

0.1
0.01

0.1
He flow rate, m3/h

1

Figure 4.	(a) Time history of the helium flow rate before andafter maintenance. (b) Relationship between normalized vibration velocity and that without bubble
and Helium flow rate.

T. Wakui, T. Naoe, H. Kogawa, K. Hanano, K. Haga, H. Kinoshita, K. Seki, T. Suzuki, and H. Ueno
Neutron Source Section, Materials and Life Science Division, J-PARC Centeri

Neutron Source

63Cryogenic Hydrogen System

2.	Development of a partitionable accumulator with a high pressure tolerance and long
cycles to failure
The temperature rise through each moderator
caused by nuclear heating for a 1 MW proton beam
operation is estimated to be 2.4 K at a circulation
flow rate of 0.19 kg/s. We prepared a heater forthermal compensation and an accumulator with bellows structure to mitigate the pressure fluctuation
caused by the proton beam on and off below theallowable pressure of 0.1 MPa.
A compact second accumulator is in use because a leakage through the welded bellows of theoriginal accumulator was identified before the cooldown operation in February JFY2010 due to a lackof weld penetration between the large diameter bellows plates. However, the present accumulator has
drawbacks, including a lower pressure tolerance(0.94 MPa) and large hysteresis during expansion
and contraction, which can decrease the numberof cycles to failure. After the summer of 2014, weplan to increase the proton beam power to reachour goal of 1 MW. We have developed a third accumulator with a higher pressure tolerance and long
failure cycle to achieve the long-term stable operation of the 1-MW proton beam.
In JFY2012, we built a prototype welded bellows
block, conducted a cycle test at a repetitive pressure variation of 2.0 MPa, and confirmed that its
cycle to failure was 14,000 cycles, which is higher
than the design value.

64

Neutron Source

The third accumulator basically adopts the samestructure and size as the second. The variable volume of the bellows required for the 1 MW proton
beam operation is also estimated to be 2.0 L. The
entire variable volume is determined to be morethan 6 L. For the third accumulator design, the plate
thickness of the welded bellows was increased from
0.4 mm to 0.8 mm to withstand a pressure of up to
2.0 MPa. Therefore, the effect of the spring constant on the pressure rise becomes larger.
The levelness accuracy was maintained within
1° throughout its manufacturing to avoid welding
distortion and excessive contact between the guidering and the guide pipe. We confirmed that the bellows can expand and contract smoothly without
hysteresis, and the gradient agrees with a design
spring constant of 76.1 N/mm, as shown in Fig.1.
Further, we adopt a new partitionable structure
to replace the accumulator more easily and shorten
the replacement process. In November of JFY2013,
the third accumulator was installed into the hydrogen loop. The accumulator was replaced in lessthan 20 days by accessing it through the maintenance hatch. This process was shortened by half,
compared with the replacement time (six weeks) required when the first accumulator had to be hoisted
to the top flange of the cold box.

Expansion fromthe maximum contraction (mm)1. Introduction
The J-PARC cryogenic hydrogen system provides cryogenic hydrogen at supercritical pressureof 1.5 MPa, with para-hydrogen concentration of
more than 99% and temperature lower than 20 K,
to three moderators generating high-performancecold pulsed neutron beams. This report describes
the topics of the cryogenic hydrogen system in
JFY2013.

100
80
60
40
20
0
-0.1

-0.05

0

Pressure difference (MPa)Figure 1. Displacement for the third accumulator.

0.05

100

300 kW

200
100

Heater power (W)

5000

70

1080 W

4000

65

3000

0.56 L

Pressure (MPa)

2000
1.55

55

1.50

1.45

60

23 kPa

0

100

200

300

400

Time (s)Figure 2. On-beam commissioning results.

The on-beam commissioning results for a
300 kW proton beam injection is shown in Fig.3.
As soon as the proton beam is injected, the pressure rises and the accumulator contracts. After the
feed-forward heater control is conducted, the pressure and temperature remain unchanged. We confirmed that the pressure rise is mitigated to 23 kPa

Hydrogen pressure
rise (kPa)300

Accumulator level(mm)Proton beam
power (kW)

400

80
60

Experimental data
Third accumulator
Second accumulator

40
Simulation result
Third accumulator
Second accumulator

20
0
0

200

400

600

800

1000

Proton beam power (kW)Figure 3.	Effect of the proton beam power on the pressure
rise.

by a bellows contraction of 0.56 L for 300 kW proton
beam power.
The pressure rise increases in proportion to theproton beam power and agrees well with its predicted value. The analytical result indicates that thepressure rise would be 60 kPa for the 1 MW proton
beam operation, which is 19% lower than that forthe second accumulator. This is because the measured spring constant for the second accumulator
becomes larger than the design value due to thelarge hysteresis. Thus, through the commissioningof the third accumulator, we confirmed that it satisfied the design requirements.

H. Tatsumoto, T. Aso, K. Ohtsu, Y. Kawakami, H. Muto, and S. Hasegawa
Neutron Source Section, Materials and Life Science Division, J-PARC Center

Neutron Source

65Modification of the MLF General Control System
for Sustainable Long-Term Operation

1. Introduction
Fig. 1 represents the outline of the General
Control System (GCS) in the MLF in 2013. It consists of several subsystems such as an integral
control system for controlling muon and neutron targets, interlock system, servers, networks, and timing distribution system. In Fig. 1, the integral control
and interlock system consists of personal computers (PC) and programmable logic controllers (PLC),
such as general control panel (GCP), local control
panels (LCP) and PPS management panel (PPSMP), which are connected through networks for
PLC links and metal cables. Their operations are
executed by monitor and operation (MO) systems
consisting of administrative control PCs (ACP), PPS
operating PC, interlock monitoring PC (IM-PC), andso on. Although the GCS has worked stably since2008, recently, the interlock and MO systems havebeen improved to ensure sustainable long- term operation and maintenance.

2. Interlock Systems
The interlock system has been modified to matchthe device upgrade of the target systems to ramp up
the proton beam power and increase the user apparatuses year after year [1]. It consists of subsystems
named MPS (Machine Protection System), TPS(Target Protection System) and PPS (Personnel
Protection System). MPS’s task is to protect animportant machine from unusual beam irradiation.
As shown in Fig. 1, after detecting the MPS signals from the LCPs, the MPS controller transmits
an “Inhibit” signal to a central control room (CCR)of the J-PARC. Then the proton beam injection into
the MLF is stopped by changing the distribution patterns of beam pulses by a scheduled timing system.
If the beam pulse is detected during emission of the“Inhibit”, the MPS signal for terminating the accelerator operation is transmitted to the CCR. The TPS
is the interlock for preventing serious troubles withthe mercury target. The TPS beam stop signal istransmitted to the CCR as “Target Status” throughFigure 1. Outline of the MLF-GCS in 2013.

66

Neutron Sourcethe PPS-MP. The 6 LCPs emit MPS signals throughmetal cables, with 3 of those LCPs also emitting
TPS signals.
The PPS is the system that prevents exposureof the personnel to high radiation by controlling theentrance into high-radiation areas (PPS areas).
The 6 PPS areas for target maintenance (TM) and
24 PPS areas for user apparatus are operated in
the MLF. The PPS-MP transmits signals to the CCR
to permit or prohibit beam injections, which are
named “Target Status”, “Safety” for safe entrance
into the PPS areas, “Emergency” for manual buttons in emergency, and “Status” for a key switch
indicating beam permission. Since the beam stop
procedure of the PPS requires high reliability, theion-source is terminated in this procedure. The IMPC collects and monitors detailed information about
the 108 MPS, 10 TPS and PPS items through the
PLC links in a lump.
3. Upgraded Full-scale MO Systems
Since 2012, we have been developing prototypes to upgrade the MO system both for the integral

control system and PPS, based on EPICS, CSS
and Postgre SQL as its framework, OPI, and server
software [2]. After confirming that they work properly, as designed, in 2013 we built two full-scale upgraded MO systems. One is the MO system, which
controls the devices for the target stations by using
more than 130 operation screens and acquires operation data about 7000 items every second. The
other is the system, which administers the PPS devices by using 6 screens and acquires data about
1400 items. They have been operated in parallelwith the current systems during beam operation andmaintenance for over half a year, and have been
debugged, unlike the current ones, which are due
to be replaced in 2014. The MO system for the PPS
was already replaced completely by the upgraded
one in the end of 2013.
References[1]	K. Sakai et al., Progress in Nuclear Science andTechnology 4 (2014) pp.264-267.
[2]	K. Sakai et al., MLF Annual Report 2012, pp.7576 (2013).

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

Neutron Source

67Scenes from the Neutron Target Station

68

Installation of octupole magnet from M1 tunnel.

Preparation of local room, called green house, with local ventilation system to prevent from contamination during replacement of the proton beam window.

Preparation for mercury discharge. Center person cut andwelded helium gas pipe with mercury.

Installation of additional shielding wall to reduce external exposure of worker in a hot cell.

Hideki Ueno, Kohei Hanano and Takashi Wakui measuring
amount of tritium in their expiration before and after mercury
discharge work.

Hideki Ueno and Toru Suzuki exchanging pressure gauges byremote handling (manipulator and in-cell crane).

Neutron SourceNeutron ScienceNeutron Science

1. User Program
In JFY 2013, the user program of neutron science has been carried out on 17 instruments(Fig. 1). The Special Environment Neutron Powder
Diffractometer − SPICA was still in commissioning phase. After completion of the commissioning
work in 2013A, BL11, the High Pressure Neutron
Diffractometer – PLANET was introduced as a public beamline to be used in the user program from
2013B.
The user program of 2013A started on April 1,2013 (Run#48) with 300 kW proton beam power.
The Elements Strategic Initiative Program and theComplementary Use Program started in the same
fiscal year. Unfortunately, the user program was interrupted during Run#49, on May 25, 2013, due tothe radiological incident at the Hadron Experimental
Facility. After the incident, all user programs, including the on-beam training of AONSA neutron schoolthat was scheduled for the 18 - 19 of June, werecancelled without carrying over. The cancelled general proposals were recommended for re-submission in the next round. On February 17, 2014, morethan eight months after the unexpected break, theuser program resumed and was ended on April 6,
2014. Since the program operated for less than twomonths, only limited numbers of general proposals
were accepted and conducted.
2. Instruments development and construction
In JFY 2013, the construction of three new instruments has progressed.
Kyoto University and KEK are installing the VIN
ROSE at BL06, which consists of a neutron resonance spin echo (NRSE) instrument and a modulated intensity by zero effort (MIEZE) instrument.
All supermirrors for neutron optical devices are deposited using the ion beam sputtering machine at
KURRI (KUR-IBS). In JFY 2013, the guide mirrors
and downstream concrete shielding were installed.

Figure 1.	Layout of the neutron instruments at MLF as of JFY 2013. Three other instruments
were under construction at BL06, 22 and 23.

70

Neutron ScienceAt BL22, the construction work of the energyresolved neutron imaging system, RADEN, continued. In JFY 2013 the shielding was completed.
Optical devices, a rotary collimator, filters and slits
were installed in the upstream position. Also, a standard shutter block of BL22 was replaced with one
specifically designed for RADEN, with three different aperture openings.
The third one, the polarized neutron spectrometer POLANO is being constructed under thejoint project between Tohoku University and KEK.
The construction of the POLANO at BL23 started
in FY2013, when the supplemental budgets wereapproved for both institutes. The basic design andconstruction of the shielding were completed, andsupermirror guides and neutron choppers were
manufactured.
Also, regular maintenance and upgrade works
have been done for the existing instruments. For
example, a beam-transport section of AMATERAS
was upgraded. At TAKUMI, a cooling system forloading experiment was completed. A 6-8 type cell
was introduced for the 6-axis multi-anvil press,
ATSUHIME at PLANET, which can allow users toreach pressure of above 10 GPa. There are also
other advancements in the beam lines, sample environments, development works on spin filters anddetectors, etc., which can be seen in individual articles in this report.

Figure 2.	Construction site at BL22 and 23 (December 25,2013). New instruments, RADEN and POLANO
were under construction.

3. Safety
After the radiological incident at the Hadron
Experimental Facility, the risk management system
of J-PARC was fully reconstructed, introducing three
response-stages to incidents, (1) Normal, (2) Alertand (3) Emergency. In MLF, whole manuals for operation and incident response were revised and several kinds of safety drills were carried out. In this report
we will introduce in brief our responsibilities for thesafety of the neutron-beam-line staff and the users.
a) Responsibility for the MLF operation and safetyof the experimental halls
Almost all of the instrumental scientists in
J-PARC and CROSS were qualified to join the Shift
Leader team as a Sub Shift Leader, which is a newly
introduced position assisting the Shift Leader, a person in charge of the MLF operation. When the Shift
Leader suspects that an event happening at the
moment jeopardizes safety, he/she declares “Alert
Stage” to stop all operations of J-PARC and proceedwith emergency calls to respond systematically tothe suspected safety violation. The Sub Shift Leader
also has the same responsibility along with the Shift
Leader. After revising the memorandum on safetyissues for the public-access neutron beam facilities
at J-PARC between the registered institute CROSS
and J-PARC, the staffs at CROSS also joined thesafety line in J-PARC as Sub Shift Leaders of MLF.
During the MLF operation period, the Shift Leader
team maintains 24-hour watch by using protection
systems and a camera monitoring system. The
quick response to any troubles in the experimental
halls will be improved by joining the teams of thebeam line staff from J-PARC and CROSS.
b) Educating and qualifying staffs in all instrumentalgroupsThe Manual for Neutron Instrument Leader has
been re-issued. All Leaders trained the members of
their instrumental group according to the manual for
the Neutron Instrument Leader and an instrumental manual, which has been revised to comply withthe revision of the upper safety regulations and theMLF operation manual. The Manager of Neutron
Experiments (Dr. Aizawa) confirmed that the instrumental group members were well trained and the

Neutron Science71Facility Manager (Dr. Arai, the MLF director) qualified them as the instrumental group staffs. For the
BL’s owned by Ibaraki Prefecture, Ibaraki Prefecture
and J-PARC agreed on a notification process for themember list of the instrumental group with confirmation of the safety response.
4. Resultant outcomes
The research activities in neutron science at
MLF resulted in more than one hundred papers.
The number includes articles in influential journals
such as Nature, Science.
We published a press release about the discovery of a new magnetic ordering phase in an ironbased superconductor LaFeAs(O1-xHx) using multiprobe analysis. The new phase was found to beformed by fine changes in the structure for x > 0.4.
This phase is adjacent to the second superconducting phase found previously in this material, but different from that in the host material (x = 0). Thus a
new host material was found, and this is expected
to be important for understanding the new mechanisms behind superconductivity.
Two staff members and one group of MLF received the 11th Japanese Society for Neutron
Science (JSNS) awards. Dr. T. Shinohara (Fig. 3)
was awarded the JSNS young researcher prize forhis work on development of the magnetic field imaging using polarized pulsed neutrons. Dr. T. Kikuchi

Figure 3.	The President of the Japanese Neutron Science
Society Prof. T. Kanaya gave Dr. T. Shinohara anaward certificate for the JSNS young researcher
prize.

was honored with the JSNS young researcher prize
for his work on the development of model-free
analysis method on quasi-elastic neutron scattering and application to liquid water. Dr. K. Nakajima,
Dr. S. Ohira-Kawamura, Dr. M. Nakamura, Dr. R.
Kajimoto and Prof. M. Arai shared the JSNS technology prize for their work on the development of achopper spectrometer with a pulse shaping chopper at a pulsed source. They received their award
certificates at a ceremony at the 13th JSNS annual
meeting held on December 12, 2013.

K. Nakajima1, Y. Kawakita1, and S. Itoh1,2
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK

72

Neutron ScienceBL01: 4D-Space Access Neutron Spectrometer 4SEASONS

1. Introduction
4SEASONS is a thermal neutron Fermi-chopper
spectrometer for inelastic scattering measurementsin the energy range of 100–102 meV [1]. The instrument has been available to users since 2009, andbecame one of the public beamlines in 2011. Now it
is stably operated by 6 instrumental scientists and1 dedicated engineer. In fiscal year 2013, 15 general proposals, including 1 trial-use proposal and 1
urgent proposal, were approved, though only 8 of
those could be conducted due to the unexpected
shutdown associated with the Hadron incident in
2013A. 3 of the 15 general proposals were requested by international users. The major research subjects are magnetic excitations in strongly-correlated
electron systems, such as superconductors andmultiferroic materials, but the number of proposals
to measure phonons in functional materials is gradually increasing.
Although the instrument operates successfully, it
still leaves room for further upgrades, and a part ofthe designed specifications has not been achieved.
Therefore, we continue to upgrade the instrument
as well as the sample environment. Here we show
examples of the major upgrades in fiscal year 2013.
2. Detectors
The vacuum scattering chamber of 4SEASONS
is equipped with 11 detector banks. Each of the detector banks can hold 32 pieces of 2.5 m-long 3He
position sensitive detectors, and the whole detectorbanks can provide scattering angle in the range of−35.3° – +130.5° in the horizontal (Fig. 1). However,
only 6 detector banks were fully occupied, resulting in the maximum scattering angle in the horizontal being only 54.5°. Increasing the number ofdetectors is one of the major issues necessary toachieve the designed specifications of the instrument, and especially important for studying phonons. Unfortunately, the recent shortage and resulting rising price of 3He gas make it difficult to install a

Figure 1.	(Top) Drawing of the vacuum scattering chamberof 4SEASONS. The orange and pink marks show
detectors which were already installed before fiscal year 2013, and installed in fiscal year 2013, respectively. (Bottom) Detector map of 4SEASONS
showing Debye-Sheller rings from a powder sample. The pink region shows the region in which thedetectors were installed in fiscal year 2013. There
are no detectors installed in the white region.

large number of detectors at once. Accordingly, weare trying to install a small number of detectors year
by year. In fiscal year 2013, we added 29 detectors (Fig. 2), which increased the maximum scattering angle in the horizontal to 68.4° (Fig. 1). We will
install more detectors in the next year to reach the
maximum scattering angle > 80°.
3. Radial collimator
To minimize scattering from the sample environment, 4SEASONS utilizes the vacuum scatteringchamber without any boundary between the sample

Neutron Science73Figure 2.	Installation of the detectors by the technical support staffs of MLF.

Figure 3.	Radial collimator being installed on 4SEASONS
by the technical support staffs.

space and the detectors. Nevertheless, the walls of
the sample environment devices, e.g. cryostat andfurnace, and the sample can inevitably produce
scattering, which contaminates the inelastic scattering data. To minimize such unwanted scattering, we recently started to use a radial collimator(Fig. 3). This collimator, which was developed by
the Technology Development Section of MLF, consists of 72 pieces of vertical blades surrounding thesample position, each of which is separated by 2.5°.
It slowly oscillates to remove the inhomogeneity inthe transmitted beam [2].
Although this brand-new device is still under test
operation, it has already been utilized for several
users’ experiments. It proved to be effective in suppressing the background from the sample environment especially in phonon measurements. One of
the biggest reasons is that acoustic phonons fromthe sample would often be overlapped by acoustic
phonons from aluminum of the sample environment
devices or a sample can because of the similarity intheir lattice constants. On the other hand, a sample
with a large dimension may not be suitable for theradial collimator, because of the low transmissionof the collimator. Users who would like to use theradial collimator are advised to consult with the instrument group prior to their experiments.
References[1]	R. Kajimoto, M. Nakamura, Y. Inamura, F.
Mizuno, K. Nakajima, S. Ohira-Kawamura, T.
Yokoo, T. Nakatani, R. Maruyama, K. Soyama,
K. Shibata, K. Suzuya, S. Sato, K. Aizawa, M.
Arai, S. Wakimoto, M. Ishikado, S. Shamoto, M.
Fujita, H. Hiraka, K. Ohoyama, K. Yamada, andC. H. Lee, J. Phys. Soc. Jpn. 80, SB025 (2011).
[2]	
M. Nakamura, Y. Kawakita, W. Kambara, K.
Aoyama, R. Kajimoto, K. Nakajima, S. OhiraKawamura, K. Ikeuchi, T. Kikuchi, K. Iida, K.
Kamazawa, and M. Ishikado, submitted to JPS
Conf. Proc.

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

174

Neutron ScienceBL02: TOF type Si Crystal Analyzer near Backscattering
Spectrometer DNA - Specification and Commissioning Results -1. Introduction
A time-of-flight (TOF) Si crystal analyzer nearbackscattering spectrometer (n-BSS), called DNA,is the first indirect geometry instrument, which uses
the coupled moderator in MLF as a pulsed neutron
source and is equipped with a high-speed pulse
shaping disc chopper, aiming for a high energy
resolution with high intensity. It aims to explore, inthe nanosecond timescale, the dynamic behaviors
of atoms and spins in bio-molecules, soft-materials,
and so on. The instrumental overview and the present specifications for DNA are shown in Table 1 andFigure 1.

Table 1. Instrumental specifications of DNA.
Items

Specification

Neutron source (NS)

Coupled Liquid H2 Moderator

L1 (source-sample)

42 [m]

L2 (sample-analyzer)~ 2.3 [m]L3 (analyzer-detector)~ 2.0 [m]Pulse sharpening chopper (PS-chopper)
Max speed: 300 Hz at ~ 7.5 m from NS(Precent Max speed: 225 Hz by 4 slits on one disc)
Crystal Analyzer
Crystal and reflection index

Si(111)Si(311) in test

Bragg angle of analyzers~ 87.5 [deg.]

Energy resolution~2.4 [meV]: Si(111) with 10 mm Slit @225 Hz~3.5 [meV]: Si(111) with 30 mm Slit @225 Hz~14 [meV]: Si(111) without PS-chopper~12 [meV]: Si(311) with 10 mm Slit @225 Hz.
Momentum range

0.07 < Q < 1.86 [A-1]: Si(111)0.60 < Q < 3.80 [A-1]: Si(311) in plan

Scan energy range:
Si(111)-40 < E/meV < 100: Single pulse scan around Ef-500 < E/meV <1500:
without PS-chopper in second frame

Si(311)-150 < E/meV <300: Single pulse scan around E f(the specifications by the end of March 2014)

Figure 1.	Overview of DNA. Each Number indicates a disc
chopper installed on the beam line BL02.

2. Construction works in 2013
Almost all spectrometer components were installed before February 2012, with the exception of
the No.1 high speed pulse shaping disc chopper. The
No.1 chopper, which is designed as a counter-rotating double-disc chopper with maximum rotationalfrequency of 300 Hz, was set up with a double-disc
during a short shut-down period in early April 2013and commissioned at 225 Hz in end of April 2013.
To evaluate the incident neutron energy distribution at the sample position, and to measure the diffraction pattern from the powder sample, three diffraction-detector-units were installed in this period.
The analyzer coverage was extended to a scattering-angle range from -18 degrees to +138 degrees
in the horizontal plain by adding some crystal analyzer units, by the end of September 2013.
3. Beam Commissioning in 2013
The commissioning started from the beginning of
February 2012. In this period, the pulse shaping highspeed chopper could not be operated, then we operated the DNA spectrometer without the pulse sharpening chopper at energy resolution of ∆E ~ 14 meVwith wide energy transfer range: -1000 < E / meV <+1500.

Neutron Science75

After installing the No.1 high speed chopper, thecommissioning of high-resolution measurement was
carried out by using single disc with slits of 10 mm
and 30 mm widths at 225 Hz in the maximum rotational speed from the end of April 2013. At this point,
the energy resolution of 2.4 μeV and 3.5 μeV withwide energy transfer range: -40 < E / meV < +100 by
one pulse scan, was achieved.
We realized an extremely low contribution of instrumental background S/N~ 105.
4.	Implementation progress of the user program in 2013A and 2013B
The user program started from May 2012. The

user program in 2013A, with 3 experiments, andin 2013B, with 3 experiments, was carried out andsome of those experiments obtained new findings,
which will be reported in near future.
Many experimental applications to the generaluser program from various scientific fields are expected in the future.
References[1]	N. Takahashi et al., Journal of Physics andChemistry of Solids 68, 2199-2203 (2007).
[2]	N. Takahashi et al., Journal of the PhysicalSociety of Japan, 80, SB007 (2011).

K. Shibata1, N. Takahashi1, Y. Kawakita1, K. Kamazawa2, T. Yamada2, M. Matuura2, T. Tominaga2, K. Nakajima1,
W. Kambara1, M. Kobayashi2, Y. Inamura1, T. Nakatani1, S. Kasai2, K. Aizawa1, and M. Arai1
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division CROSS-Tokai76

Neutron ScienceCurrent Status of IBARAKI Biological Crystal DiffractometeriBIX at BL03

1. Current Status
The IBARAKI biological crystal diffractometer,
called iBIX, is a high performance time-of-flightneutron single crystal diffractometer designed toobserve mainly the hydrogen, protonation and hydration structure of biological macro molecules andthen to elucidate the basic mechanism of catalytic
reaction and drug development based on the 3-dimensional molecular structure.
Starting from the end of 2008, iBIX with 14 detectors was made available for users’ experiments
supported by Ibaraki University [1]. In 2012, wecompleted the installation of 30 new detectors forthe iBIX diffractometer (Fig. 1) [2]. The new iBIX is
expected to become one of the world’s best-performing neutron single crystal diffractometers forbiological macro molecules. Since January 2013,
the new iBIX has been available regularly to users’
experiments for protein samples. The final specifications of the iBIX is shown in Table 1.
In FY2013, 3 organic compounds and 5 biological macromolecules were provided to the diffraction experiments by using iBIX. From these analyses, some scientifically interesting results could

be obtained by using the characteristic of neutron
structure analysis (eg. Observation of hydrated water related to catalytic reaction;possibility of new reaction mechanism).

Figure 1. The iBIX Diffractometer.

Table 1. The final specifications of the iBIX.

Moderator
Guide tube (m)L1 (m)
L2 (m)
Max. unit cell length (Å3)
Measurement region in dspacing (Å)
Range of neutron wavelength (Å)
Neutron flux (neutrons/sec/cm2)
Sample environment
Detector
Size of sensitive area (mm2)
Spatial resolution (mm)Standard size of sample (mm3)Standard measurement time (days)

Coupled H2 (para) 100 × 100 mm2
25
40
0.49
~ 13530.35 < d < 50
0.5 < λ < 9.0 or more
7 × 107
Gas flow type cooling system, He: ~20 K, N2: ~90 K
Two-dimensional, scintillator, wavelength shift fiber type
133 × 133
Less than 1
1
0.5 for Organic compounds
3 for Biological macromolecules

Neutron Science77

2. Development
In FY 2013, we prepared users manual and distribution package of the data reduction software“STARGazer” which will allow the iBIX users themselves to perform data reduction in their laboratory.
At the same time, we held a software workshop for
iBIX core users.
Some components of the data reduction software have been upgraded and newly developed inorder to become a software system able to processdata faster and in a more friendly way. For example,
visualization components of peak search reflections
were newly developed to check the peak search results. The component of data format conversion andstatistics calculation was prepared to be applied forthe structure analysis by users.
As of the hardware, we installed the new dataacquisition system, which has faster data reading
and writing function and larger storage than the previous one (Fig. 2). Also the pulse laser system was
prepared as part of the utility equipment for sample
environment and multi-purpose stage was developed to mount the utility equipment for sample environment with the sample (Fig. 2).
3. Feature prospects
In the future, the accelerator power of J-PARC
will be improved at 1000 kW. The data reduction software should be upgraded continuously inorder to become more user friendly and be available for samples with large unit cell and/or smaller
volume for measurement of full data set. The wide
pulse shape in TOF direction of coupled moderator
and large unit cell of the samples cause overlap of
the adjacent Bragg spots. Next year, we will start
to develop the peak profile fitting method in orderto improve the accuracy of the data reduction for
the integrated intensities of Bragg reflections andto realize the method to de-convolute overlappingreflections.

Figure 2.	(a) New data acquisition system (b) multi purpose
stage and (c) laser sysytem.

As of the hardware, we should prepare the utility equipment for sample environment (e.g. heatingand extension) and a fast and friendly measurement system before the accelerator power reaches
1 MW.
References[1]	I. Tanaka, K. Kusaka, T. Hosoya, N. Niimura,T. Ohhara, K. Kurihara, T. Yamada, Y. Ohnishi,
K. Tomoyori and T. Yokoyama, Acta Cryst. D66(2010) 1194–1197.
[2]	K. Kusaka, T. Hosoya, T. Yamada, K. Tomoyori,
T. Ohhara, M. Katagiri, K. Kurihara, I. Tanaka
and N. Niimura J. Synchrotron Rad. 20 (2013)
994–998.

K. Kusaka1, T. Hosoya1, T. Yamada1, T. Ohhara2, M.Katagiri1, I. Tanaka1, and N. Niimura1
1
Frontier Research Center for Applied Atomic Sciences, Ibaraki University, Tokai; 2Neutron Science Section, Materials and Life Science
Division, J-PARC center78

Neutron Science

Study of the Energy Resolution of the Pulsed Neutron Beam
Provided by ANNRI (BL04)

1. Introduction
The ANNRI (BL04) at J-PARC/MLF was constructed in order to measure the neutron capture
cross-section as a function of the neutron energy inthe thermal and epithermal neutron energy regions.
The neutron energy resolution is important to ensure the quality of the cross-section data. The neutron energy is calculated by the time-of-flight (TOF)
method. The TOF resolution is composed of thetwo factors: the time structure of the incident proton
beam to the mercury target of the JSNS and thetime uncertainty due to the neutron slowing-down
process in the liquid hydrogen moderator. We studied the neutron energy resolution by simulation calculation, in which the above two factors were taken
into account, and measurements of the time resolutions in the thermal and epithermal neutron energy
regions.
2. Simulation
The simulation of the neutron slowing-down process was performed using the Monte-Carlo code
PHITS [1]. The procedure is almost the same as
explained in the reference [2]. At the JSNS, theincident proton beam is normally delivered in a

double-bunch scheme and the time interval between the two bunches is 599 ns. Each bunch also
has time width of 60 ns under the JSNS operation of
17.5 kW. We convoluted the time structure obtainedby the simulation with the time structure originatingfrom the proton beam and show the neutron pulse
in Fig. 1. This Figure shows the relation between
the time and energy at the moderator surface. In
the case of the double-bunch mode, the pulse splits
into two below about 10 eV. This is due to the double-bunch scheme and indicates that we need totreat this property carefully at analyzing experimental data obtained at ANNRI. Fig. 2 shows the time
width in FWHM obtained by the data in Fig. 1. The
time width is the same, below about 10 eV for both
single- and double-bunch modes. The double-bunchmode approaches about 600 ns as the neutron energy increases. On the other hand, the single-bunchmode does about 60 ns. We calculated the energy
resolution at the sample position (L = 21.5 m) on thebasis of the time width in Fig. 2 and show it in Fig. 3.
The energy resolution is almost equal or less than
1% below 100 eV. However, the energy resolution
for the double-bunch mode deteriorates drasticallyas the neutron energy increases.

Figure 1.	Two-dimensional plots of the time and energy of neutrons at the moderator surface. The time structure of
the proton beam is taken into account. (a) and (b) are the results for the single- and double-bunch modes,
respectively [3].

Neutron Science

79

10

FWHM (µs)

103Single bunch
Double bunch

2

10
1
10-1
10-2

10

-3

10-2

10-1

1

10

102

10

3

104

10

5

10

6

Neutron Energy (eV)Figure 2.	The FWHM values for the time structure by thesimulation as a function of neutron energy. The
solid and dashed lines represent the single- anddouble-bunch modes, respectively [3].

∆E/E at L=21.5 m

10Single bunch
Double bunch

1

10-1

10

-2

10

-3

10

-3

10

-2

10

-1

1

10

10

2

10

3

10

4

10

5

10

6

Neutron Energy (eV)Figure 3.	
Neutron energy resolution at 21.5 m from themoderator based on the simulation. The solid anddashed lines represent the single- and doublebunch modes, respectively [3].

3. Measurements
We performed measurements of the time widthof neutron pulses at the thermal and epithermal
neutron energy regions using different methods.
In the thermal neutron energy region, we applied
the diffraction method using a Mica sample. The sample was set at 28.5 m from the moderator in the beamline. Diffracted neutrons were detected by a He-3
neutron detector set at an angle of 162° with respect
to the beamline downstream. Fig. 4 shows observed
neutron pulses and comparison with the simulation
calculation. The observed pulses consist of fast andslow components and these are perfectly reproducedby the simulation calculation. These two components
can be represented by slowing-down and storage
terms of the model function proposed by Ikeda andCarpenter [4]. We obtained pulse width in FWHM byfitting the pulses using the above model function.

80

Neutron Science

In the epithermal neutron energy region, we applied resonances of the neutron capture reaction by
Ta-181 at the single-bunch operation of the JSNS. A
tantalum foil with a thickness of 0.1 or 0.01 mm wasset at 29.54 m from the moderator in the beamline.
Prompt gamma rays associated with the neutron
capture reaction were detected by a plastic scintillation detector and the TOF data was recorded. Fig. 5
is the TOF spectrum obtained by the 0.1-mm thicksample. A lot of resonances were observed at theneutron energy indicated by the nuclear data library
JENDL-3.3 [5]. We fitted 17 resonances by the function, which was obtained by the convolution of the
intrinsic resonance shape expressed by the singlelevel Breit−Wigner, the neutron pulse expressed by
the model function proposed by Ikeda and carpenter, the time structure of the proton beam, and the
Doppler effect of Ta-181 nuclei. The widths of neutron pulses were obtained from the fit results.
4.	Comparison of the simulation and measurements
Fig. 6 shows a comparison of the measurements
and the simulation calculation. They are in agreement for the absolute value and trend dependingon the neutron energy. This result means that the
JSNS and ANNRI work properly. Furthermore, thesimulation is reliable for deducing pulses in energy
regions, which the measurements cannot access.
5. Conclusions and future prospects
The simulation and measurements of neutron
pulses of the pulsed neutron beam at ANNRI were
performed. They showed good agreement, which
implies the reliability of the simulation calculation.
The simulation revealed the energy resolution of
ANNRI and the necessity for a special treatment for
the neutron-capture cross-section data in the caseof a double-bunch mode of the JSNS.
In this work, the neutron pulse was studied for
the JSNS condition of 17.5 kW. The JSNS poweris expected to become 1 MW in near future. The
property of the neutron pulse may change by an increase of the JSNS power. Therefore, the pulse has
to be checked by simulation and measurement on acontinuing basis for precise analysis of the neutron
capture cross-section data.

10-2

0.76 meV

1.7 meV

3.1 meV

6.9 meV
10-3

10-6
76000

76500

77000

10-4

10-5

51000

51500

52000

10-6
38000

52500

TOF (µs)

39000

10-3

10-4

10-5

40000

TOF (µs)

Intensity (n/µs/pulse)

10-5

10-6

77500

TOF (µs)

10-4Intensity (n/µs/pulse)

10-5

Intensity (n/µs/pulse)

10-3

10-4

Intensity (n/µs/pulse)

Intensity (n/µs/pulse)

4.8 meV

10-2

10-3

30500

31000

31500

TOF (µs)

10-4

10-4

26000

26500

27000

TOF (µs)

28 meV

Intensity (n/µs/pulse)

10-5

23 meV

Intensity (n/µs/pulse)

10-4

10-3

25500

10-3

19 meV

10-3

Intensity (n/µs/pulse)

Intensity (n/µs/pulse)

Intensity (n/µs/pulse)

10-3

15 meV

10-5

10-6

32000

10-3

12 meV

10-4

10-4

10-5

10-4

10-5

10-5
10-6
19000

19500

10-5

20000

TOF (µs)

17000

17500

10-6
13800 14000 14200 14400 14600

15200 15400 15600 15800 16000

TOF (µs)

TOF (µs)

10-6

TOF (µs)

12800

13000

13200

TOF (µs)

13400

10-3

32 meV

37 meV

62 meV

10-4

10-5

Intensity (n/µs/pulse)

Intensity (n/µs/pulse)

Intensity (n/µs/pulse)

10-4

10-5

10-5

10-6
11800

12000

12200

TOF (µs)

10-4

10800

11000

11200

TOF (µs)

11400

8450

8500

8550

TOF (µs)

8600

8650

Figure 4.	Comparison of measured diffractions (data points) with the time structures obtained by the simulation (solid lines). The
value indicated in each figure corresponds to the neutron energy of the diffraction. The dashed and dotted lines are theslowing-down and storage terms in the model function proposed by Ikeda and Carpenter, respectively [3].

103

Measurement (Thermal)

413 300

200

10Neutron Energy (eV)
40
20
10

100

1.673

Measurement
Evaluated cross section

1
-1

10

FWHM (µ s)Intensity (1/ µ s/pulse) or Cross section (arb.unit)

Measurement (Epithermal)

102

Simulation (Single bunch)

10

1

10-2
-3

10

10-4
10-5

10-1
2

1.05×10

2

2×10

2

4×10
TOF (µs)238×10 103

1.65×10Figure 5.	Measured TOF spectrum with the thick tantalum
foil and the cross-section of the neutron capture reaction based on the nuclear data library
JENDL-3.3 at a temperature of 300 K [3].

-3

10

10-2

10-1

1

10

Neutron Energy (eV)

102

3

10

Figure 6.	Comparison between the simulation and measurements of the FWHM values of the time structures of neutron pulses for single-bunch mode [3].

Neutron Science81

Acknowledgements
The present study is the result of “Study on nuclear data by using a high intensity pulsed neutron
source for advanced nuclear system” entrusted to
Hokkaido University by the Ministry of Education,
Culture, Sports, Science, and Technology ofJapan (MEXT). This work was supported by JSPS
KAKENHI Grant no. 22226016.

References[1]	K. Niita et al., PHITS: Particle and Heavy Ion
Transport Code System, Version 2.23, JAEAData/Code 2010-022, 2010.
[2]	K. Kino et al., Nucl. Instrum. Methods Phys.
Res. A626 (2011) 58.
[3]	K. Kino et al., Nucl. Instrum. Methods Phys.
Res. A736 (2014) 66.
[4]	
S. Ikeda and J.M. Carpenter, Nucl. Instrum.
Methods A239 (1985) 536.
[5]	K. Shibata et al., J. Nucl. Sci. Technol. 39(2002) 112.

K. Kino1, M. Furusaka1, F. Hiraga1, T. Kamiyama1, and Y. Kiyanagi2 on behalf of the ANNRI collaboration
1
Faculty of Engineering, Hokkaido University; 2Graduate School of Engineering, Nagoya University

82

Neutron Science

Studies of Neutron Optics for Physics Researches

1. Introduction
At the NOP beamline (Neutron Optics andPhysics) installed at the port BL05, the final preparation for neutron lifetime measurement, as well assome other researches and developments are continuing. The detailed analysis of commissioning data
showed that certain challenges should be resolved.
The time projection chamber (TPC) to detect neutron beta decay was upgraded to suppress background events and electric noises effectively. The
UCN accelerator was improved to accept a wide
range of neutron velocity. The simulation study forneutron scattering experiments to search middlerange force also progressed. Apparatus including
gas target and scattering chamber was designed
for the experiment at NOP.

Figure 1.	
Typical event display for 3He capture (top) andbeta decay (bottom). They can be identified by deposit energy and track geometry.

2. Commissioning for neutron lifetime measurement
The recent values of neutron lifetime deviate far
beyond the systematic errors claimed in the pastand require further improvement to ensure consistency with the primordial Big Bang nucleosynthesis.
We are continuing the neutron lifetime measurement at the polarized beam branch of the NOP
beamline installed at the port BL05 [1]. The system consists of a neutron chopper (SFC) and a gas
chamber (TPC) for detecting the electrons from theneutron beta decays [2]. The TPC contains small
amount of 3He. The rate of the 3He(n,p)3H reaction
is measured by counting the protons. The neutron
lifetime is measured as the ratio of the electron
events to the proton events. The detailed analysis
of commissioning data told us some problems to beresolved. The TPC was upgraded to suppress background events and electric noises effectively.
We clearly observed neutron beta decay eventsand 3He capture events in the commissioning
data. Now we are checking the analysis procedure
carefully.

3. UCN optics upgrade
Ultra Cold Neutrons (UCNs), which are neutrons
with velocity of less than 7 m/s, are used mainlyfor particle physics. To get dense UCNs at the experimental position, the optical system “rebuncher”
for neutron focusing was already demonstrated[3]. We improved the rebuncher to accept a wide
range of neutron velocity so that the range of frequency of RF spin flipper for acceleration of UCNs
was twice as large as previously demonstrated. The
RF power was also increased for flipping efficiency.
Now we are preparing the focusing experiment byusing Doppler shifter on NOP [4]. We also develop
a new type of neutron mirror for UCN guide tubes
using deuterated diamond-like carbon film. A mirror with optical potential of 243 neV was fabricatedsuccessfully by the CVD method [5], which has anadvantage to deposit inner surface. It is quite important to estimate the motions of UCNs to discuss thesystematics in high precision experiments. We havealso developed simulation tools based on GEANT4
to treat UCN’s motion [6].

Neutron Science83

4.	Precision measurement of scattering from
window material
A measurement of angular distribution of scattering cross section is planned for the search of
unknown medium range interactions between neutrons and neutral atoms. We confirmed that the
total cross section of silicon as a window material
measured at NOP was in good agreement with thetheoretical prediction. The simulation studies also
advanced. The experimental apparatus, including
gas target and scattering chamber, was designed
based on the results of the simulations. Now we arepreparing the experiment with full-setup at low divergence beam branch.
References[1]	T. Ino et al., J. Phys.: Conference Series 528(2014) 012039.
[2]	
H. Otono, Dr. Sc. Dissertation (University ofTokyo, 2012).
[3]	Y. Arimoto et al., Phys. Rev. A 86 (2012) 023843.
[4]	K. Mishima et al., J. Phys.: Conference Series
528 (2014) 012030.

Figure 2.	Measured total cross section by Silicon block as afunction of the neutron wavelength. The blue solidline shows a theoretical line obtained by Freund et al.

[5]	D. Sakurai et al., J. Phys.: Conference Series
528 (2014) 012010.
[6]	R. Katayama et al., J. Phys.: Conference Series
528 (2014) 012031.

Y. Arimoto1, T. Ino2,3, S. Muto3, K. Taketani2,3, H. Oide4, T. Yoshioka5, H. Otono5, T. Yamada6, K. Mishima6, S. Yamashita6,
H. Sumino7, S. Imajo8, Y. Iwashita8, M. Yamada9, Y. Seki9, Y. Otake9, Y. Yamagata9, P. Geltenbort10, K. Hirota11,
M. Kitaguchi11, H. M. Shimizu11, T. Shima12, H. Funahashi13, K. Asahi14, and Y. Kiyanagi15
1
Accelerator Laboratory, KEK; 2Neutron Science Section, Materials and Life Science Division, J-PARC center; 3Institute of Materials Structure
Science, KEK; 4CERN; 5Department of Physics, Kyushu University; 6International Center for Elementary Particle Physics, University ofTokyo; 7Department of Physics, University of Tokyo; 8Institute for Chemical Research, Kyoto University; 9RIKEN; 10Institut Laue Langevin;11
Department of Physics, Nagoya University; 12Research Center for Nuclear Physics, Osaka University; 13Institute for Liberal Arts and Science,
Kyoto University; 14Department of Physics, Tokyo Institute of Technology; 15Faculty of Engineering, Hokkaido University

84

Neutron Science

Advance Neutron Beam Line for VIllage of Neutron
ResOnance Spin Echo Spectrometers (VIN ROSE) at BL06

Kyoto University and KEK are jointly installing
two types of neutron spin echo (NSE) spectrometers at BL06, that is, a neutron resonance spinecho (NRSE) instrument and a modulated intensity
by zero effort (MIEZE) instrument. The NSE technique is an essential spectroscopic method, which
has achieved the highest neutron energy resolution
at the present moment. NSE with a pulsed neutron
source makes it possible to scan very efficiently
wide spatiotemporal space. We named the beamline “VIN ROSE” (VIllage of Neutron ResOnanceSpin Echo spectrometers), which will spawn a new
field of spectroscopic methods [1].
In Figure 1, the schematic top view of BL06
beam line is shown. Both NRSE and MIEZE makeuse of neutron resonance spin flippers, which madeit possible to design and install compact and multiple spectrometer machines in a narrow space.
Another characteristic is the adoption of two curved
guides rolling to create experimental space for two
spectrometers and transport optimized neutron
beams. By using the curved guide tubes, fast neutrons and gamma rays from the source are stopped
by an iron beam dump at the upstream part of the
instruments.

NRSE is suitable to study slow dynamics ofsoft condensed matter with high energy resolution,
while MIEZE has a big advantage of flexible sample
environments with potential to open new fields ofstudy such as spin dynamics in strongly correlated
systems. In Table 1, the planning instrumental specifications of VIN-ROSE are listed.
The neutron optical devices are key componentsof the spectrometers. Some of the devices, such as
focusing mirror and related devices have been developed and improved step by step. All the supermirrors for these guides are deposited on silicon wafers
with thickness of 3 mm by using the ion beam sputtering machine at Kyoto University (KUR-IBS) [1, 2].
The supermirrors are held precisely and covered byiron shields to reduce the dose level. The NRSE andMIEZE guides use Qc = 2.5 and 3 supermirrors, respectively. Their high performance has been provenby neutron reflectivity measurements, etc.
In FY2013, the guide mirrors and the downstream concrete shielding were installed, and the
instruments’ commissioning has been started in
FY2014. Figure 2 shows a picture of BL06 and theobserved beam profiles with neutron imaging plate
for the instruments.

Figure 1. Schematic top view of MIEZE and NRSE beam line at BL06.

Table 1. Planning instrumental specifications of VIN-ROSE.

Spectrometer

Wavelength

Q range [Å-1]Fourier Time

MIEZE

3 < λ < 13 [Å]

0.2 < Q < 3.5

1 [ps] < t < 2 [ns]NRSE

5 < λ < 20 [Å]

0.02 < Q < 0.65

0.1 [ns] < t < 0.1 [μs]Neutron Science

85

(a)

(b)

(c)

Figure 2.	Picture of BL06 (a), observed neutron beam profiles for NRSE (b) and MIEZE (c), by
neutron imaging plates, respectively.

References[1]	M. Hino, T. Oda, M. Kitaguch, N. L. Yamada,
H. Sagehashi, Y. Kawabata, H. Seto, Physics
Procedia 42 (2013) 136.

[2]	M. Hino, H. Sunohara, Y. Yoshimura, R. Maruyama,
S. Tasaki, H. Yoshino and Y. Kawabata., Nucl.
Inst. Meth. A 529 (2004) 54.

H. Endo1,2, M. Hino3, T. Oda3, N. L. Yamada1,2, H. Seto1,2, and Y. Kawabata3
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3Kyoto
University Research Reactor Institute86

Neutron ScienceUpgrade of SuperHRPD

1. Introduction
The super high resolution powder diffractometer
SuperHRPD suffered damage by the Great East
Japan Earthquake on the 11th of March 2011. The
first stage of the restoration works had been carriedout until March 2012. The beam time for the generaluser program started from April 2012 and all of theresearch proposals for fiscal year 2012 had beensuccessfully conducted. The incident in the hadron facility happened at the beginning of FY 2013,
which caused slight delay in the second stage of therestoration works that had been scheduled for thesummer.
As part of the upgrade of the instrument, a new
detector system of 8 mm diameter position sensitive
detectors (PSDs) were installed at the backward
detector bank and the number of detectors of the
90 degree bank was increased. The data acquisition system was completely changed to new computers and data storages.
2.	Restoration works of the re-alignment of theguide tube and improvement of the beam line
shielding
The earthquake caused optical deviation in theguide tube system. A complete restoration of thesystem was carried out during the beam shut down
period in the summer of FY 2013. In this alignment
work, the vacuum jacket of the guide tube and theguide tube support system were improved at thesame time. The iron vacuum jackets of the curved
guide section in the upstream were replaced withaluminum jackets. The lower weight of these aluminum jackets (Figure 1) simplified the support system. At the straight guide section without vacuum
jacket in the downstream, about 50 m of the guidetube support system was also changed to aluminum, which made it lighter.
The beam line shield of the straight guide section
was completely redesigned to concrete containing
boron (Figure 2). The former beam line shield had a

Figure 1.	New aluminum vacuum jackets. One unit is about
2 m in length and a support pillar is installed ineach unit.

Figure 2.	New design of the beam line shield of the straightguide section. Concrete containing boron is used.

small clearance of a few cm around the guide tube.
Since the earthquake caused deviation of the optical axis, it was necessary to adjust not only theguide tube but also the beam line shield. The new
design of the beam line shield has a ten-odd cm
clearance around the guide tube, which does not
require adjustment and a large move of the shieldat the time of re-alignment of the guide tube.
3.	New detector system with 8 mm diameter position sensitive detector
Because of the insufficient initial budget and thedelay of development in the high spatial-resolution

Neutron Science87detector system, we initially installed 1/2 inch diameter position sensitive detectors (PSDs) that had
been used at KENS facility of KEK. This imposed
limit on the resolution compared with the designed
one. Then we developed a new detector system
based on 8 mm diameter PSDs and improved theresolution as shown below. The 16 PSDs with diameter of 8 mm were composed together into one unit
and an amplifier circuit was connected to each PSD.
In the new detector system, 8 amplifier circuits werebuilt into one application specific integrated circuit(ASIC) chip and this made the circuit more compact(Figure 3).
The test measurement using the new detector
system was performed in May 2013. In this measurement, four new detector units were arranged at
the backward detector bank to cover the area of 2θ
= 157° ~ 172°. A diamond powder sample enclosed
in a sample holder of 6 mm in diameter was used.
We were able to obtain a very sharp diffraction peakshown in Figure 4 with ∆d/d = 0.0637%. Since theresolution of the normal sample with the 1/2 inch
PSDs system is about ∆d/d = 0.1%, it is evident
that the improvement of the resolution has beenachieved by the 8 mm PSDs system. All detectorsof the backward bank of SuperHRPD were replacedwith this new detector system during the beam shut
down period in the summer of FY 2013.

8 mm PSD (4 Boxes - 64 PSDs)
Sample : diamond powder φ 6 mm

40×103intensity / arb.unit

Figure 3.	The conventional amplifier circuit (left) and the advanced one with an ASIC chip (right); the 16 amplifier circuits are accumulated in two ASIC chips.

Fitting function : squared Lorentzian
Resolution ∆ d/d = 0.0637%

30

20

10

0

0

20

40

60

TOF / msec

80

100

120

61.20

61.25

61.30

61.35

TOF / msec

61.40

Figure 4.	Neutron diffraction pattern of a diamond powder sample using the new detector system (left).
The peak fitting result by squared Lorentzian function (right).

S. Torii1,2, M. Yonemura1,2, and T. Kamiyama1,2
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK

88Neutron ScienceDevelopment of an Advanced Special Neutron Powder
Diffractometer under Extreme Environment for Materials

1. Introduction
The demands of batteries as energy storage
have increased with the advancement of the technologies for compact and portable devices such as
laptop computers and mobile phones. Additionally,
hybrid vehicles (HV) and pure electronic vehicles(EV) using high performance batteries are designed
to reduce the consumption of fossil fuels and contribute to the realization of a low carbon society.
The lithium ion battery is a promising battery system candidate as energy storage for both small andlarge cells. However, the lithium ion battery is still
under development to resolve the issues of cyclic
life and high temperature use. Its capacity is also
limited and needs to be improved.
The lithium ion battery works by lithium ion transfer between cathode and anode. The reactions ofboth electrodes are based on the de / intercalationof lithium ion from / into the materials of electrodes.
When the lithium ions intercalate into material, thecrystal structure changes. The information about
the structural change of the electrode and the location of lithium ions in the crystal structure leads toimprovements in the present lithium ion battery andthe invention of an out-of-the-box battery.
In order to clarify at an atomic level the structures of cathode, anode and the interface between
electrode and organic electrolyte, a new neutron
powder diffractometer, SPICA, has been designed
and constructed as one of the state-of-the-art measurement apparatuses. In comparison with X-ray,
the neutron is well known to be a more powerfulprobe to get information about the location andmovement of light elements such as hydrogen andlithium atoms. Therefore, the advantage of neutron
diffraction will allow us to acquire more knowledge
about the location and movement of lithium ions aswell as the change of the atomic arrangement in thecathode, anode and electrolyte solution.

2. Present status
Several reference materials such as Si, CeO2 andTiO2 provided by the National Institute of Standards
and Technology (NIST) were measured to confirm
the reliability of the SPICA instrument. Figure 1
shows the typical diffraction data from the referencematerial, NIST TiO2 powder, using all banks. All diffraction profiles indicated low background and goodsignal-to-noise ratio. A typical measurement time
was 0.5 hr for 0.5 g of NIST Si powder at 25/3 Hz
repetition.

Figure 1.	Diffraction profiles of the TiO2 powder at low angle,
90° angle, high angle and back scattering banks.

Figure 2 shows the Rietveld refinement patternsof CeO2 collected by back scattering and 90° banks.
The observed intensities are consistent with those
calculated from the structure model, which indicatesthe capability and reliability of the diffractometer. In

Neutron Science89

d spacing / Å

(a)

(b)

5

Cathode material

5

4Anode material

4

3

3

discharge

charge

2

1

2

0

360

720

1080

1440

Discharged time / min.

Figure 2.	Rietveld refinement pattern of NIST CeO2 on
SPICA. Observed (red +), calculated (solid light
blue line) and difference (dark blue line) data areplotted. (a) Back scattering banks and (b) 90ºbanks (air scattering chambers).

addition, SPICA gives expectation of structure refinement by in situ measurement. Figure 3 showsa typical example of in situ measurement for acommercialized Li-ion battery (LIB). The high capacity cell with nominal capacity 3000 mAh was
charged and discharged between 4.25 and 2.5 V
at currents of 0.1 A in constant current - constantvoltage (CC-CV) charging and in constant current(CC) discharging. In situ neutron diffraction data
were collected under cycle rates of 1/30 C in discharging and charging processes. The structuralchange of the material, which is dependent on thelithium content, is clearly observed. The lattice parameters for the anode and cathode materials as afunction of the lithium content were extracted from

1
1800
0

360

720

1080

1440

1800

Charged time / min.

Figure 3.	The changes of diffraction profiles in an 18650-type
lithium battery as a function of discharge / chargetime.

the diffraction pattern. The structure refinement is inprogress. This promising result shows that SPICA
has a high potential of structure refinement for insitu measurement.
The commissioning of the SPICA diffractometeris still continuing. Simultaneously, various kinds oftest measurement using conventional samples havebeen carried out by the NEDO project members.
Acknowledgements
This work was supported by the Research andDevelopment Initiative for Scientific Innovationof New Generation Batteries (RISING) projectof the New Energy and Industrial Technology
Development Organization (NEDO). The neutron
scattering experiment was approved by the Neutron
Scattering Program Advisory Committee of IMSS,KEK (Proposal No. 2009S10).

M. Yonemura1,2, T. Fukunaga3, K. Mori3, T. Kamiyama1,2, M. Nagao2, Y. Ishikawa2, S. Torii1,2, Y. Onodera3, R. Tomiyasu2,
H. Asano2, T. Sakuma4, T. Ishigaki5, A. Hoshikawa5, K. Aizawa1, S. Harjo1, K. Kino6, R. Kanno7, M. Hirayama7, Y. Idemoto8,
N. Kitamura8, H. Arai9, and Y. Uchimoto10
1
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3Research
Reactor Institute, Kyoto Univ.; 4Insitute of Appl. Beam Sci., Ibaraki Univ.; 5FRC, Ibaraki Univ.; 6Graduate School of Eng. Hokkaido Univ.;
7Interdisciplinary Graduate School of Sci. and Eng. Tokyo Institute of Tech.; 8Faculty of Sci. and Tech., Tokyo Univ. of Science; 9RISING
Project, Kyoto Univ.; 10Graduate School of Human and Environmental Studies. Kyoto Univ.

90

Neutron ScienceBL10: NOBORUIn FY 2013, 9 general use proposals were carriedout at NOBORU, but three of them have not been
completed due to the Hadron incident on May 23.
This year, we planned to study temporal changes inneutronic performance before and after the replacement of the Mercury target at the long-shutdown period, but unfortunately we failed to do it. During the
shutdown period, we performed remodeling of thebeam-line components.
A temporary light shutter, composed of 10 cm
thick polyethylene and 2 cm thick 6LiF tile, has beenused in the experimental room of BL10 to prevent
radioactivation of the imaging camera during datatransportation time. The light shutter was installedat permanent position in the beam transport sectionof BL10 in November. It also works as a filter, which
high-energy neutrons and γ-rays penetrate. A beam
duct in the beam transport section, shown in theFig.1, was also replaced by the new one at the sametime. The new duct has a cross section of 112 mm2with a Gd2O3 painted scrapers opening of 100 mm2.
The old duct has a cross section of 100 mm2, whose
inner surface reflects cold neutrons significantly.

These undesirable neutrons will be absorbed by thescrapers of the new duct.
Periodical measurement
To investigate neutronic performance as wellas to keep JSNS in optimum operating conditionin J-PARC, we periodically measured the neutron
spectra at BL10 in the several conditions of instrumental devices, such as rotary collimator, B4C
slits, and so on. Figure 2 shows an example setting
for the periodical measurement at BL10. Figure 3
shows the neutron spectra measured by the samesettings in May, 2013 and in Feb., 2014. The proton beam power in each measurement was about
300 kW. The hole size of rotary collimator and adjacent aperture size of B4C slit 1 were changed between (a) and (b), whereas the other settings were
the same in each experiment. A little difference inthe neutron intensity was observed after normalization. The energy-dependent attenuation ratio would
be attributed to the increased air path of 1.1 m after
the remodeling of the beam-line components.

Figure 1. Picture of the beam line components of BL10 at around 8 m position.

Neutron Science91Figure 2. Beam-line components of BL10 and the collimation setting for the periodical measurement.

Figure 3. Measured neutron spectra in May, 2013 and Feb. 2014 in different collimation setting.

References[1]	M. Harada et al., to be submitted to Proceedingsof the J-PARC Symposium 2014.

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

92

Neutron ScienceBL11: High-Pressure Neutron Beamline PLANET Opened
for General Users

1. Introduction
The PLANET is the beamline dedicated for highpressure diffraction experiments. The constructionof the beamline was completed in JFY 2012, andthe beamline was opened to general users from
JFY 2013. Here, we report on recent results anddevelopments we are working on now.
The beamline has a high resolution and wide accessible d-range enough to conduct structure analysis of crystalline and liquid materials [1-2]. The severe
incident and receiving collimators make it possible toobtain the signal only from the sample surrounded bymany materials, such as a sample container, heaterand pressure transmitting medium. Appreciating
those benefits, many users from various sciencefields are now coming to use the PLANET (Fig. 1).

Figure 1.	Statistics of the users from various science fields
from 2013 to 2014.

2. Typical example
Structure analysis of crystalline materials
Figure 2 shows the temperature dependenceof the neutron diffraction patterns of portlandite
Ca(OD)2 at 3 GPa. Thanks to the radial collimators, no contamination from a sample container anda heater was observed and all the peaks were assigned as portlandite. The quality is high enough to
conduct Rietveld analysis. The detailed results fromthe structure analysis will be shown elsewhere.

Figure 2.	Temperature dependence of the diffraction patternof Ca(OD)2 at 3 GPa.

Structure analysis of amorphous materials
The PLANET offers the opportunity to investigate the structure of the amorphous and liquid materials under high pressure. To test the feasibility,
we took the data for SiO2 glass. First, we checked
the consistency between our ambient data and thewidely accepted one, and confirmed it. Figure 3
shows the structure factor at high pressures up
to 10 GPa obtained after several corrections. The
pressure dependence indicates marked changes
in the intermediate range order, which is consistent
with the previously reported high-pressure behavior. The details will be shown elsewhere.

Figure 3.	Pressure dependence of the structure factor S(Q)of the SiO2 glass up to about 10 GPa.

Neutron Science933.	Extension of the accessible PT-conditions
using 6-8 type cell
The 6-6 type cell has been used successfully inthe 6-axis multi-anvil press (ATSUHIME), but theavailable PT conditions were limited to below 10 GPa
and 2000 K. To extend the accessible PT range, weapplied a 6-8 type cell assembly to ATSUHIME. The
cell consists of eight second-stage anvils, gaskets
and a furnace assembly (Fig. 4). The cubes of a SiC
sintered diamond with truncated edge length (TEL)of 5 mm were used as the second stage anvils,
where the initial volume of the sample was 6 mm3.
We tested the pressure generation using aninternal pressure standard of NaCl, and confirmed
the generation of 16 GPa at 1600 kN based on theequation of state of NaCl (Fig. 5). The heating test
was also conducted at up to 1273 K at 1600 kN.
During the heating to 1073 K, the pressure was decreased to 14 GPa due to the relaxation of the gasket materials. The 6-8 type cell allows us to investigate the structure of the material under the pressureof above 10 GPa. Figure 6 shows an example, thediffraction pattern of CaSiO3 perovskite that is one of
the major components of the Earth’s lower mantle.
This phase is stable only at pressures above 14 GPa
and unquenchable to ambient condition, thus the

Figure 4. Photograph of a 6-8 type cell and schematic drawings of the furnace assembly and the second stage anvil.

Figure 5.	Pressure generation curve for a 6-8 cell with TEL of 5 mm. The horizontal axis is the load applied to the bottom ram.

94

Neutron ScienceFigure 6.	Diffraction pattern of CaSiO3 perovskite obtained at 15.4 GPa with a 6-8 cell. The
tick marks show the calculated peak positions for the cubic CaSiO3 (cyan), MgO(orange) and LaCrO3 (purple). The stars indicate the peaks that can be indexedwith the orthorhombic cell.

in-situ experiment is necessary. Previous X-ray diffraction and theoretical studies showed that theunit cell is not cubic, but the detailed crystal structure is yet to be revealed. In this study, the calcium
perovskite was successfully synthesized from thestarting material of wollastonite under pressure bykeeping it at 1373 K for 3 hours. The diffraction was
taken at 15.4 GPa for 36 hours after the temperature
decreased to room level. We found marked peaks,
which had not been observed in the previous x-ray
studies, thanks to the different scattering length of
Ca, Si and O for neutrons. Those are indexed withan orthorhombic cell, and the detail refinement of thecrystal structure is now in progress.

References[1]	
H. Arima, T. Hattori, K. Komatsu, J. Ab, W.
Utsumi, H. Kagi, A. Suzuki, K. Suzuya, T.
Kamiyama, M. Arai, and T. Yagi, J. Phys. Conf.
Ser., 215 (2004) 023025.
[2]	T. Hattori, A. Sano-Furukawa, A. Yamada, H.
Arima, W. Utsumi, H. Kagi, MLF Annual Report,(2012) 96–97
Acknowledgement
Authors thank to Dr. Nagai for kindly offering thedata of portlandite.

T. Hattori1,2, A. Sano-Furukawa1,2, K. Funakoshi3, J. Abe3, and S. Machida3
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Quantum Beam Science Center, JAEA; 3Neutron R&D
Division CROSS-Tokai

Neutron Science95

High Resolution Chopper Spectrometer at BL12

1. Introduction
The High Resolution Chopper Spectrometer(HRC) is being operated at BL12 to study dynamics in condensed matters with high resolutions using relatively high energy neutrons. A research project using the HRC is being conducted to observe
wide range of correlated electron systems. We performed experiments concerning these subjects andintroduced instrumental improvements.
2. Instrumentation
An experimental control environment was developed to combine the measurements of neutron
counts with the control of devices such as choppers, temperature controllers, goniometers, vacuum system, and so on, as shown in Fig. 1 [1]. The
HRC Control Platform was developed and installedon the computer named DAQ-OP (DAQ operator).
The HRC Device Control Software controls the devices as well as the DAQ middleware (DAQ MW)
via Control LAN through the Platform. The HRC
Experiment Control Software executes a sequence
composing begin/end of measurements and controls of devices. At present, almost all the deviceson the HRC can be controlled through this platform
and their operations connected with the data acquisition (begin/end of measurements). In order to optimize the computing environment, the compositionof the computers was improved.
We also developed software to analyze single
crystal sample data as well as powder sample data.
The analyzed data can be transformed to the standard Mslice format for convenience of the users.
The process for alignment of the sample crystal
became very easy. The excitation spectra in thethree-dimensional system on the four-dimensionalenergy-momentum space can be also measured byrotating the sample crystal axis, and visualized.
In order to cool down the sample stably, a GMtype refrigerator was installed. This refrigerator
shows a good cooling performance by improving the96

Neutron Science

Figure 1.	Experimental control environment on HRC. PMC,
TC, GPIB-ETH represent a pulse motor controller,a temperature controller, a GPIB/Ethernet converter, respectively. The vacuum system is accessible
through the Gateway server and the FL-net. The
incident neutron beam is controlled by the Fermi
chopper and the narrower, and the sample environment such as the temperature and the crystal
angle is controlled. The operation status of the T0
chopper and the vacuum system is monitored.

radiation shielding, and we have confirmed that thelowest temperature available by using this refrigerator is 3 K. A cryomagnet to apply a magnetic field of
up to 14 T to the sample was designed, manufactured and delivered. We started the commissioningat the Guide Hall of JRR-3M, and confirmed that it
was successfully operated with the maximum magnetic field of 14 T.
During the partial mounting of the new PSDs, avacuum leakage occurred in March 2014. To findthe leakage point, all the thin Al windows were removed and replaced by thick plates, because of thesafety regulations. The low angle detectors mounted outside the vacuum were removed. Fortunately,
the leakage points were at the vacuum connectionsof PSDs, not at the Al windows. At present, although
the high vacuum has been recovered, the low angle detectors mounted outside the vacuum are3. NBS Experiments
NBS is an advantageous method for observing
coherent excitations in non single-crystal materials. Owing to the kinematic constraints of neutron
spectroscopy, incident neutron energy in the subeV region with a high resolution is necessary, andthe scattered neutrons need to be detected at very
low scattering angles, for measuring scattering in
the forward direction near (000). On the HRC, thebackground reduction at low angles down to 0.5°
successfully showed that the NBS method was
feasible. As we previously reported, spin waves ina polycrystalline ferromagnet La0.8Sr0.2MnO3 (TC =316 K) observed on the HRC well agreed with theprevious result from the single crystal sample, as
shown in Fig. 2(a). This shows the feasibility of the
NBS on the HRC.
The spin waves in a polycrystalline ferromagnet,
SrRuO3 (TC ~ 160 K), were similarly measured. For
this material, a large single crystal suitable for inelastic neutron scattering experiments has not yet
been synthesized. As shown in Fig. 2 (a), the spinwave dispersion relation was well fitted to E = E0 +DQ2 with an apparent energy gap E0. The possible
reason for this characteristic feature is an induced
spin anisotropy from a spin-orbit coupling acting on
the Ru 4d orbital.
Nd2Fe14B is a well-known strong permanent
magnet, and all spins are aligned along the c*-axis
at room temperature. In a previous inelastic neutron
scattering experiment using a single crystal, a spinwave branch was detected only along the c*-axis
around (002). We performed NBS experiments ina Nd2Fe1411B polycrystalline sample at room temperature. The observed peak positions were on thedispersion curve along the c*-axis reported in theprevious experiment (Fig. 2(b)).
Phononic excitations in a liquid D2O were measured at room temperature on the HRC. The excitation peaks showed broad energy spectra. The
observed dispersion relation well agreed with thatfor the fast sound observed in the previous experiment at Q ≥ 0.35 Å-1 using a steady state neutron
source. The experiment on the HRC extended thedata points to the lower Q (Fig. 2(c)).
10

15
(a)

E (meV)

still removed. However, the PSDs for the neutron
Brillouin scattering (NBS) experiments are mounted
in the vacuum and operational.

15
(b)
11
Nd2Fe14 B
T = 300 K

La0.8Sr0.2MnO3
T = 245 K
SrRuO3
T=7K

(c)
D2O
T = 300 K

10

10

5

5

5

0
0.0

0.2

0
0.4 0.0

0.2

0
0.4 0.0

0.2

0.4

0.6

-1

Q (Å )

Figure 2.	Dispersion relations obtained by the NBS experiments on the HRC: spin waves in La0.8Sr0.2MnO3and SrRuO3 (a), spin waves in Nd2Fe1411B at 300 K(b), and phononic excitations in D2O at 300 K (c).
The blue solid lines are determined by previous
experiments. The dashed line in (a) is a fitted
curve to E = E0 + DQ2 with constants E0 and D.
The solid black lines are the upper boundary accessible by using conventional spectrometers withthe lowest angle of 5°.

References[1]	S. Itoh, T. Yokoo, D. Kawana, H. Yoshizawa,
T. Masuda, M. Soda, T. J. Sato, S. Satoh, M.
Sakaguchi and S. Muto, J. Phys. Soc. Jpn. 82
SA033 (2013).
[2]	S. Itoh, T. Yokoo, D. Kawana, Y. Kaneko, Y.
Tokura, M. Fujita, K. Yoshida, K. Saito, N.
Inami, Y. Takeichi, K. Ono, Y. Endoh, J. Phys.:Conf. Series 502 012043 (2014).

S. Itoh1,2, T. Yokoo1,2, T. Masuda3, H. Yoshizawa3, M. Soda3, Y. Ikeda3, S. Ibuka2, T. Asami3, R. Sugiura3, D. Kawana3,
T. Shinozaki3, and Y. Ihata4
1
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3The Institutefor Solid State Physics, The University of Tokyo; 4Technology Development Section, Materials and Life Science Division, J-PARC Center

Neutron Science97

BL14 AMATERAS

1. Introduction
AMATERAS (Fig. 1) had five staff members
after Dr. Chiba-Kamoshida joined as outsourcing
staff in April 2013, which resulted in more substantial user support after eight months of the beam-off
period of J-PARC. We made efforts to improve theinstrumental activities, such as an upgrade of thebeam-transport section and on-beam commissioning of several new devices as mentioned below. It
should be also reported here that two works related
to AMATERAS received awards from the JapaneseSociety for Neutron Science (JSNS), namely the development of a chopper spectrometer with a pulseshaping chopper at a pulsed source by Dr. Nakajima
et al. (Fig. 2) and the development of a model-free98

Figure 1. Photo of AMATERAS (in September, 2013).

analysis method on quasi-elastic neutron scatteringand its application to liquid water by Dr. Kikuchi [1].
2. Instrumental activities
In JFY2013, the following instrumental activities
were carried out: 1) commissioning of sample environment devices, 2) replacement of defective components and 3) upgrade of components. Also, regular maintenance of components and regular performance tests were carried out as routine works.
12 days of instrument-group-use beam-time werespent for on-beam parts of the above activities.
In the beginning of 2013A, an operation test ofa BL-common 7 T cryomanget on AMATERAS was
carried out (Fig. 3). Magnetic fields of up to 4 T weresuccessfully achieved. Since we were concernedthat the scattering chamber of AMATERAS, which
is made of steel, might cause serious damage tothe magnet due to magnetic force, we did not try toapply an even higher field. As we expected, hugebackground from the outer vacuum chamber, radiation shields and a support ring for the magnet
was observed. Still we could observe a field dependence of magnetic excitations in a powder sample
by subtracting background data obtained from anempty scan.
During the long shutdown period of MLF, thebeam-transport section was upgraded (Fig. 4). The
discrepancy between the intensity expected from

Figure 2. Photo of the award ceremony at the JSNS meeting.

Figure 3. A BL-common 7 T cryomanget on AMATERAS.

Neutron ScienceAs with the other major instrumental activities,
replacement of a defective detector tube, installing a Cd film attenuator, and background reduction
study were done in JFY 2013.

Figure 4. Re-alignment of AMATERAS beam-transport.

simulation and that observed in real measurements
was one of the serious problems of AMATERAS.
Misalignment of guide tubes and performance of apart of mirrors had been suspected to be the sourceof this problem. Therefore, we replaced the mirrors (8.6 m in length) and re-aligned full-part of thebeam-transport. The performance after this upgrade
was checked in the 2013B period. The intensity became 1.2 times larger in a low-energy region (Ei <5 meV) and nearly twice in a high-energy region(Ei > 80 meV) compared to the previous intensity.
However it is still lower than the simulated intensity.
We continue our investigation, including checking
the validity of the simulation.

3. User Program
There was a wide variety in the research fieldsof the proposals on AMATERAS. In the 2013A and2013B periods, 14 general use proposals were accepted, and six proposals were listed on the reserved subjects. We also accepted two project use
proposals, which are ‘Study of structure and electronic properties of functional materials at BL14’ (PI:T. Masuda) and ‘Project research on structure anddynamics of protonic, superionic and amorphous
functional materials using AMATERAS’ (PI: Y.
Inamura), and one element strategy use proposal,‘Neutron-scattering research on element-strategy
project for electronic materials’ (PI: Y. Murakami).
Due to the incident at the Hadron Experimental
Facility, five general use experiments were cancelled or interrupted. The beamtime for the project
use and element strategy use experiments werealso reduced.
Reference[1]	T. Kikuchi et al., Phys. Rev. E 87, 062314(2013).

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

Neutron Science99Upgrading of TAIKAN and Needs of the Users

The small and wide angle neutron scattering instrument TAIKAN (BL15) has been developed andupgraded to analyze microstructures or hierarchicalstructures of substances in various scientific fields
precisely and efficiently with a 1 MW spallation neutron source in J-PARC. In FY2013 these activities,
user support, and research activities were done at
TAIKAN by the staff shown in Fig. 1, as well as byother staff.
The detector system of TAIKAN is composed of 5detector banks: the small-, middle-, high-, ultra-smallangle, and backward detector banks. On the smallangle detector bank in a vacuum scattering chamber, 128 3He PSD tubes were additionally installed.
The numbers of 3He PSD tubes then increased to760, 304, 104, and 48 for the small-, middle-, highangle, and backward detector banks, respectively.
Figure 2 shows a photo of the small-angle detectorbank after installing the 3He PSD tubes.
The software for data analysis was newly developed by Y. Inamura and T. Ito, et al. in order to solve
completely the problems with the reliability and efficiency of the previous software. Figure 3 shows
one of the windows of the new software. The window shows a 3D image of the detector arrangement
and scattering data of a standard sample, silver
behenate.

Figure 1. Group photo of the staff in charge of TAIKAN.

100

Neutron Science

Figure 2. Photo of the small-angle detector bank.

Figure 3.	3D image of the detector arrangement and scattering data drawn by the new software. The datashows the scattering from a standard sample, silver behenate.

A T0 chopper was installed just downstream of
the first disk chopper in order to suppress the highenergy neutrons and γ-rays generated at the neutron source. The rotational frequency of the chopper
is usually 25 Hz, but 50 Hz can also be chosen.
Figure 4 shows the statistics of the application
for using TAIKAN in the period from 2011B to 2014A.
In the scientific field of the application, “Soft matter,
Chemistry” is the most numerous at 45%. There areother scientific fields with high percentages, whichare “Electronic, Magnetic”, “Structural”, “Biology,
Life”, “Environment, Energy”, and “Instrument”,
where “Structural” denotes structural materials suchɫɼʍʏʄɾʇʀ
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ɔɀɠʉʑʄʍʊʉʈʀʉʏɇ
ɠʉʀʍʂʔ
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direction or perpendicular to it.
Figure 6 shows a photo of a tensile load cell forthe experiment of soft matters. A sample can be set
inside a gas chamber. The initial interval between
two chucks is 10 to 15 mm. The stroke is less than
100 mm. The tensile force is 1 N to 1 kN. The head
speed is 0.01 to 100 mm/min. The temperature of thesample can be controlled between RT and 300oC.

Figure 4.	The scientific applications proposed to TAIKAN in
the period from 2011B to 2014A.

as steels, “Environment, Energy” denotes battery
and catalyst materials, and “Instrument” denotes
the development and upgrading of TAIKAN. Most
SANS users are international users in the scientificfield of “Soft matter, Chemistry”. However, among
the applicants of TAIKAN, the percentage of those
involved in other scientific fields is also high. This
seems to reflect applicants’ needs for precise andefficient analysis of microstructures or hierachicalstructures of substances with TAIKAN.
In order to respond to the needs of users in various scientific fields, an electromagnet and a tensile
load cell were introduced.
Figure 5 shows a photo of a 0.2Tesla-electromagnet for the experiment of electronic and magnetic substances. In order to cool a sample, a4K-cryostat can be installed between the coils of
the electromagnet. A horizontal magnetic field canbe applied to the sample either along the beam

Figure 5. Photo of a 0.2Tesla-electromagnet.

Figure 6. Photo of a tensile load cell.

J. Suzuki1,2, S. Takata1, K. Ohishi2, H. Iwase2, T. Tominaga1,2, T. Morikawa2, M. Sahara2, T. Hosoya1, Y. Inamura1, T. Ito2, T.
Nakatani1, T. Shinohara1, T. Oku1, K. Suzuya1, K. Aizawa1, M. Arai1, T. Otomo1,3, and M. Sugiyama4
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division, CROSS-Tokai; 3Institute of Materials
Structure Science, KEK; 4Research Reactor Institute, Kyoto University

Neutron Science101Development of Sample Environments of SOFIA Reflectometer
for Seconds-Order Time Slicing Measurement

Neutron reflectometry (NR) is very useful for investigations on structures of surfaces and buriedinterfaces composed of soft materials. A beam line
(BL) 16 in J-PARC/MLF is dedicated for a horizontal
type neutron reflectometer. At BL16, two downward
neutron beams (2.22° and 5.71°) are transported
from a coupled hydrogen moderator to irradiate freesurface such as air-water interface. In order to realize a neutron reflectivity measurement with a highflux neutron beam at J-PARC/MLF as early as possible, we started to accept the neutron beam with
“ARISA-II” reflectometer relocated from the KENS
facility in 2008 [1]. However, the motion range ofthe slits, sample and detector stages were so shortthat only the 2.22° beam line at BL16 was used, because the components of ARISA were not designed
for this beam line. This is a serious disadvantage
in an air-liquid interface measurement to observehigh-q region with a high incident angle.
To overcome this problem, ARISA-II was replaced with a brand-new reflectometer “SOFIA(SOFt-Interface Analyzer)” in 2011 through the collaboration between JST/ERATO and KEK [2, 3].
Figure 1 shows a schematic drawing of SOFIA in
the experimental hutch. With the new slit, sample,
and detector stages, we can accept the 5.71° beamline as well as the 2.22° beam line. This enables
us to measure NR over wide scattering vector (q)region on free liquid surfaces. Also, the slit system
can finely collimate to irradiate an area of 10 mm ×
10 mm, a typical sample size for synchrotron lightsources, with an angular resolution of 3%.
SOFIA reflectometer normally utilizes a white
neutron beam with a wavelength band of 0.2 nm to
0.88 nm with repetition of 25 Hz produced by pulsed
proton beam of J-PARC, in which the wavelength canbe evaluated by a time-of-flight method using the relationship of a wavelength and mass of de Broglie wave:
λ=

h ,
mv

where λ, h, m, and v are the wavelength, Planck’s
constrant, mass, and velocity, respectively. Using
this method, we can scan a wide momentum transfer q(= 4πsinθ/λ) at a time in a reflectivity profile,even with a fixed incident angle of neutron θ. Thisis the big advantage for time-slicing measurement
because reflectivity profile with wide-q data can beacquired without any angle scan. For extending
the q-region, SOFIA equips double frame mode inwhich the wavelength band of 0.2 nm to 1.76 nm
is available by chopping every two neutron pulses.
In order to take full advantage of wide wavelengthband of SOFIA, we developed sample environments for time-slicing measurement: one is for solid-liquid contact measurement and the other one isfor temperature-jump measurement.

Figure 1. Side view of SOFIA reflectometer placed at BL16 in J-PARC/MLF.

102

Neutron ScienceFigure 2 shows a photograph of a sample cell fora solid-liquid contact measurement. A sample substrate with 3 inch in diameter is packed with a tub
made of a borosilicate-glass. The tub has two apertures: one is to inject liquid and the other is for an air
vent. The liquid sample in a container falls down by
opening the electromagnetic valve, and then gets incontact with the sample substrate. To avoid evaporation of the liquid, the liquid container is connectedwith the air vent. This way, the liquid can be introduced remotely after sample position alignment.
Figure 3 shows a photograph of a sample cellfor temperature-jump measurement. 100 W IR laser
is introduced into an evacuable chamber through a
rod and magnifying lenses to homogenize and magnify the laser, respectively. The size of the laser at
the sample position is 2 inch in diameter, in which
the sample is irradiated with the laser from the backside. The temperature of the sample is measured
by a radiation thermometer, and the laser power isregulated by a PID controller. This way, the laser
can be turned on remotely after sample positionalignment.
First, we performed test workings with thesesample cells and confirmed that both system canchange the environments within 10 seconds. Next,

Figure 2.	Photograph of a sample cell for a solid-liquid contact measurement.

Figure 3.	Photographs of a sample cell for a temperaturejump measurement.

we actually performed time-slicing measurementswith phospholipid multi-layer on a Si substrate incontact with heavy water for a solid-liquid contact
measurement, and with thin film of deuterated polystyrene on a Si substrate for a temperature-jumpmeasurement. The test experiments were successfully done, and remarkably, the accumulation time of
20 seconds was enough in both cases [4].
In the future, the beam current of J-PARC will be
upgraded to 1 MW, over 3 times higher than now.
Moreover, we are planning to upgrade a detector
that have high efficiency and count rate. These enable us to shorten the accumulation time by tentimes, that is, second-order time slicing measurement will be available. Then, the sample environments developed in this study will play an essential
role in achieving that.
References[1]	K. Mitamura et al., J. Phys. Conf. Ser. 272(2011) 012017.
[2]	N. L. Yamada et al., Euro. Phys. J. Plus 126(2011) 108.
[3]	K. Mitamura et al., Polymer J. 45 (2013) 100.
[4]	N. L. Yamada et al., in preparation.

N. L. Yamada1,2, K. Mitamura3,4, N. Torikai5, H. Sagehashi2, S. Sato2, H. Seto1,2, T. Oda6, M. Hino6, M. Furusaka7, and
A. Takahara3,4
1
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3JST, ERATO,
Takahara Soft Interfaces Project; 4Institute for Materials Chemistry and Engineering, Kyushu University; 5Graduate School of Engineering, Mie
University; 6Research Reactor Institute, Kyoto University; 7Department of Quantum Science and Engineering, Hokkaido University

Neutron Science103

BL17 Polarized Neutron Reflectometer, SHARAKU

1. Introduction
Neutron reflectometry is now widely recognized
as an indispensable technique for development of
nanotechnology and investigation in the field of surface and interface sciences. The polarized neutronreflectometer SHARAKU, named after the famous
Japanese ukiyo-e printer, was installed at BL17 as
the second reflectometer of the MLF.
SOPHIA, the first MLF reflectometer, constructed at BL16, can measure neutron reflectivity fromthe free surface and interface because BL16 is abeam line that delivers neutron beams downwards.
On the other hand, BL17 is a normal horizontal
beam line. Thus we designed SHARAKU as a polarized neutron reflectometer with vertical sample
geometry.
The construction of SHARAKU was completed
in the beginning of 2012, and then we started thecommissioning and a small portion of the user program. Now SHARAKU is widely open to international users. However, we have been improving the reflectometer and making it user-friendly. In this article
we report the progress achieved in this fiscal year.
2. Installation of a new vacuum chamber
We installed a new vacuum chamber in between
a sample position and a detector bank. The chamber is composed of two cells along the beam line,
and each cell has an elevator as shown in Fig. 1. Anelectromagnet to keep the neutron polarization isset on the elevator in the upstream cell, and a spin
flipper and a spin analyzer are set on the elevatorin the downstream cell. These elevators enable us
to quickly and safely switch between the two setups
for polarization and non-polarization analysis mode.
We had to use a crane to mount and dismount the
spin analyzer, and it took almost an hour without theelevators. But now the switching time is reduced to
five minutes and all we have to do is to push a button on a touch panel of a controller. Figure 2 shows
this new chamber.

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Neutron Science

Figure 1.	Cross sectional view of the newly installed vacuum chamber.

Figure 2.	A picture of SHARAKU with the newly installedvacuum chamber and a multi-wire type position
sensitive chamber (MWPC). This picture was taken at the detector side (downstream of the beamline).

3.	Installation of a two-dimensional position
sensitive detector
At the end of the 2013B term the main detectorof BL17 was a 3He tube without position sensitivity.
We have prepared three types of two-dimensional(2D) position-sensitive detector (PSD) for a varietyof advanced reflectometry applications, such as offspecular reflection, grazing incidence small-angle
neutron scattering (GISANS), and grazing incidence
diffraction (GID) measurements.

The first is a multi-wire type position-sensitive
proportional chamber (MWPC). This detector has
better spatial resolution than other detectors, highcounting-rate, and high efficiency. The second is a
2D scintillation detector using a wavelength-shiftingfiber (WLSF) readout. The effective area is 256 mm
× 256 mm with 4 mm × 4 mm spatial resolution. The
last one is a scintillation detector based on a position-sensitive photomultiplier. The effective area is
100 mmϕ in diameter with 0.5 mm × 0.5 mm spatial
resolution.
The performance of these detectors was evaluated using a DAQ system of BL17, and it was confirmed that all detectors performed satisfactorily as
expected. Figure 3 displays a GUI panel for analysis of the 2D data obtained by the 2D-PSDs.
References[1]	M. Takeda et al., Chinese J. Phys. 50 (2012)161.
[2]	K. Toh, T. Nakamura, K. Sakasai, K. Soyama,and H. Yamagihshi, J. of Phys.; Conf. Ser. 528(2014) 012405.

Figure 3.	Two-dimensional intensity map of an incident anda reflected neutron beam and their profiles along
two diagonal directions extracted from data taken
by a multi-wire type position-sensitive chamber(MWPC).

M. Takeda1,2,3, D. Yamazaki2, K. Soyama2,3, K. Aizawa2, M. Arai2, Y. Inamura2, T. Nakatani2, S. Sakasai2, K. Toh2,
H. Yamagishi2, T. Nakamura2, N. Miyata4, M. Mizusawa4, K. Akutsu4, S. Kasai4, and M. Katagiri5
1
Quantum Beam Science Center, JAEA; 2Materials and Life Science Division, J-PARC Center; 3Department of Research Reactor and Tandem
Accelerator, JAEA; 4Neutron R&D Division, CROSS-Tokai; 5Frontier Research Center for Applied Atomic Science, Ibaraki University

Neutron Science105

BL18: Current Status of SENJUSENJU is a TOF single-crystal neutron diffractometer designed for precise crystal and magnetic
structure analyses under multiple extreme environments such as low-temperature, high-pressure andhigh-magnetic field, and also designed for taking
diffraction intensities of small single crystals withless than 1.0 mm3 down to 0.1 mm3 in volume.
In 2013, we added 6 area detectors, and determined the accurate and precise parameters for all
area detectors by using basic diffraction method ofa standard sample. In addition, we carried out diffraction measurements of Zr-based bulk metal glass
to evaluate it as a material of piston-cylinder typehigh pressure cell.
1. Addition of 6 area-detectors
For a single crystal diffractometer, covering alarge area around the sample position is very important to reduce the measurement time for one
sample. After the launch of SENJU in March 2012,
SENJU had been operated with 31 wavelength shiftfiber (WLSF) type scintillation area detectors [1].
SENJU was originally designed to have 37 area
detectors. In April 2013, we added 6 detectors asshown in Fig.1. Three of them were set on a backscattering detector bank (S1: 2θ = 157.5 deg), andFigure 1.	Arrangement of area detectors at SENJU (topview). 3 detectors were added to the S1 bank andother 3 to the S5 bank.

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another three were on a low angle detector bank
(S5: 2θ = 45.0 deg). Diffraction measurements of aruby single crystal showed that the efficiency anduniformity of the new 6 detectors were similar to
those of the original 31 detectors.
2.	Determination of accurate and precise detector parameters
The instrumental parameters, including the positions of the detectors and the neutron flight path
length, were determined in order to obtain accuratelattice parameters of the samples. Since the instrumental parameters correlate with each other, seriesof different measurements were needed to obtainthe unique values for each parameter. As the firststep of the procedure, a powder diffraction patternof diamond was measured to determine the scattering angle of 90 deg utilizing the nature of the DebyeSheller ring, which lines up vertically at 90 deg. On
this measurement, we determined the actual 2θ angle of the 90-deg detector. Simultaneously, we determined the total neutron path length from the neutron source to the detector of the 90-deg bank (L1 +
L2). As a next step, a Bragg reflection was repeatedly measured as the sample crystal was rotatedin small steps. From this data, the equatorial planeparameters and the distance between the sample
and the detectors L2 were determined for the detectors settled at the horizontal plane. Consequently,
the equipment parameters of the 90-deg detector
were precisely determined without using any material constant. As a third step, many Bragg reflections from a standard sample were measured by thestep scan of the crystal. This measurement gives
a unique reciprocal lattice using the 90-deg detector. Then, the positions of the Bragg reflections ofother detectors were adjusted so that the positionalparameters of each detector were determined. As aresult, the lattice parameters can be obtained withthe accuracy of about 0.05% using the determined
instrumental parameters.

3. Evaluation of bulk metal-glass as a material
for high-pressure cell
For single crystal neutron diffraction measurements under high pressure, the piston-cylinder typesample cell has an ideal geometry because the apparatus has a wide opening accessible direction
for incoming and scattered neutrons, if the cylindermaterial is transparent enough for neutrons. As amaterial for the new piston-cylinder cell, we havefocused on the Zr-based bulk metallic glasses (ZrBMGs), which have ideal properties as a cylindermaterial in terms of exceptional tensile strengths,
plasticity, no sharp Bragg peaks and transparency
for neutrons.
Neutron diffractions for a cast rod of Zr-BMG witha diameter of 12 mm and a length of 15 mm, which
will be used as a cylinder material and the empty
piston-cylinder made of CuBe alloy with outer/innerdiameters of 8.8/2.5 mm as a reference were measured at SENJU. It was confirmed that the Zr-BMG
is amorphous; no sharp Bragg peaks were found in
the pattern (Fig.2 (a)), except a broad hallow ring.
On the other hand, lots of peaks with a slight texture
were observed for CuBe cylinder (Fig.2 (b)).
4. User program
Three general proposals were conducted in
2013A, and four general proposals in 2013B. In addition, four project uses were also carried out.

Figure 2.	Comparison of neutron diffraction for (a) a rod of Zr-BMG and(b) an empty cell made of CuBe, measured at SENJU.

T. Ohhara1, R. Kiyanagi1, T. Kawasaki1, K. Oikawa1, I. Tamura1,2, K. Kaneko1,3, A. Nakao4, T. Hanashima4, K. Munakata4,
T. Moyoshi4, T. Kuroda4, Y. Kawamura4, Y. Noda1,5
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Department of Research Reactor and Tandem Accelerator,
JAEA; 3Quantum Beam Science Center, JAEA; 4Neutron R&D Division, CROSS-Tokai; 5HANARO, KAERI

Neutron Science107Engineering Studies at BL19-TAKUMI

1. Introduction & present status
Regretfully, TAKUMI had to cancel many excellent proposals for the 2013A period due to the
HADRON incident. The TAKUMI team is also thankful that the users resubmitted their proposals forthe 2013B period. Many excellent experiments withvarious kinds of materials covering residual strain
mappings and various kinds of in situ measurements while loading at room temperature, low andhigh temperatures, have been conducted.
TAKUMI operated approximately 75 days during
2013 FY and the beam time allocation according toexperiment type is shown in Figure 2. The percentage of strain mapping is almost unchanged while
the in situ studies increased compared to 2012 FY.

2. New sample environments
A new sample environmental device, the 100 K
cooling system for loading experiments (Figure 3),
has been commissioned and is ready to be usedin the user program. The 100 K cooling system forloading experiments is a compact vacuum chamber equipped with loading specimen jigs; it can bemounted on the standard 50 kN loading machineof TAKUMI. The temperature of specimen jigs canbe set in a range from 77 K to 473 K with an accuracy of about ± 1 K by controlling liquid nitrogenflow and heater power. The standard specimen
shape is a dog bone type cylinder for tension and/or
compression.

Figure 1.	TAKUMI team performs alignments of the sample
positions and theodolites routinely.

Figure 3.	Illustration (up) and photo (bottom) of the 100 K
cooling system for loading experiments.

Figure 2.	
Beam time allocation by experiment type at
TAKUMI during 2013 FY.

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3. Selected topics
There are many excellent results from experiments done during 2013 FY, and also excellent
publications in 2013 FY. We regret that only three
topics will be briefly introduced here, while the topics about the high elastic strain in Fe3Pt [1] and theAxial strain

Lateral strain
Lates(a) Axial

D10

D50
D10

Internal strains in ITER CS conductor [3,4]Measurements of internal strains in the superconducting constituent (Nb3Sn phase in Nb3Sn strand)in two cable-in-conduit conductors (CICC) for theInternational Thermonuclear Experimental Reactor
were performed. From the internal strain measurements in a CICC for the central solenoidal magnets
after the similar performance test, in the full-size
shape as used in the performance test (3.6 m long)and in 100 mm long cut bars. Three main results
were obtained. (1) The residual strain difference before and after the cutting to 100 mm long bar was
about 0.1%, (2) a large relaxation on residual thermal strain was observed at the high field zone, and(3) the large relaxation on residual thermal strain at
the high field zone was found mainly in a cross-sectional side where the Lorentz force coming in.

bond resistance between rebar and concrete is an
important parameter for determinig its performanceand it has been typically evaluated by measuring
the strain distribution along the embedded rebar.
Here we present an in-situ strain and stress measurement for the rebar in the reinforced concrete
using time-of-flight neutron diffraction as a novel
alternative technique to the typical strain gauges.
It was demonstrated in this study that the three-dimensional deformation behavior of the embedded
rebar in normal-strength concrete, cured in air, canbe accurately measured under pull-out loading using time-of-flight neutron diffraction.

D50

strengthening mechanism of advanced steel (TRIP)[2] are introduced in different chapters of this report.

(b) Lateral

Figure 5.	Internal strain distributions in rebar embedded
in concrete measured at external stresses of
33 MPa, 125 MPa and 250 MPa. The absolutevalues of lattice strains in the axial direction and in
the lateral direction, are linearly increased towards
the end of the bonding region (x = 0). Portions
where the changes in the lattice strain occur correspond to anchorage zones, and its lengths are
increased with increasing the external stresses,
followed by increases in the lattice strain at thebonding region.

Figure 4.	Internal strains of Nb3Sn phase for the axial direction and the history of external field during the
SULTAN test. The internal strain is shifted from theaverage strain to the tensile side (and peak broadening is also observed) at the LLS of the HFZ by
the cyclic test.

Internal strains in rebar embedded in air-cured
concrete [5]In the modern society, architectural and civil engineering structures such as reinforced concretebuildings require high seismic performance to minimize the “megarisk” exposure to urban earthquake
hazards. In the reinforced concrete structures, theTensile behaviors of newly developed LPSO MgZn-Y alloys [6]The tensile behavior of single-phase 18R-Long
period stacking ordered structure (LPSO) Mg-Zn-Y
alloys and two-phase Mg-Zn-Y alloys which consistof Mg matrix and 18R-LPSO phase were studied byin-situ pulsed-neutron diffraction technique under tensile stress. Anisotropic behavior between the a-axis
and c-axis in the 18R-LPSO structure was observed
for the single-phase LPSO Mg-Zn-Y casted alloy fromthe elastic region under tensile stress. On the other
hand, two-phase Mg-Zn-Y alloys with low 18R-LPSO
phase concentration, which were produced by

Neutron Science109

extrusion, have isotropic behavior until the yield point
under tensile stress, and the 18R-LPSO phase acts
as a strengthening phase in the plastic region.

Figure 6.	Tensile behavior of the as-cast Mg85Zn6Y9 in the axial direction. Lattice strains for (6060) and (00018)
planes indicate those being parallel to the a-axis
and the c-axis, respectively, while lattice strains for(42 28) and (42 2 10) indicate those being non-parallel to both the a-axis and the c-axis. The latticestrains seem to have nearly linear relation to themacroscopic stress until the specimen was broken.

References[1]	T. Yamaguchi, T. Fukuda, T. Kakeshita, S. Harjo
and T. Nakamoto, Appl. Phys. Lett. 104 (2014)
231908.
[2]	S. Harjo, N. Tsuchida, W. Gong, J. Abe, K.
Aizawa, Mater. Res. Soc. Symp. Proc. 1528
(2013).
[3]	
T. Hemmi, S. Harjo, Y. Nunoya, H. Kajitani,
N. Koizumi, K. Aizawa, S. Machiya and K.
Osamura, Supercond. Sci. Technol., 26 (2013)
084002.
[4]	S. Harjo, T. Hemmi, J. Abe, W. Gong, Y.
Nunoya, K. Aizawa, T. Ito, N. Koizumi, S.
Machiya, K. Osamura, Mater. Sci. Forum, 777(2014) 84–91.
[5]	H. Suzuki, K. Kusunoki, Y. Hatanaka, T. Mukai,
A. Tasai, M. Kanematsu, K. Kabayama and S.
Harjo, Meas. Sci. Technol., 25 (2014) 025602.
[6]	K. Aizawa, W. Gong, S. Harjo, J. Abe, T.
Iwahashi, T. Kamiyama, Mater. Trans., 54(2013) 1083–1086.

S. Harjo, K. Aizawa, T. Kawasaki, W. Gong, and T. Iwahashi
Neutron Science Section, Materials and Life Science Division, J-PARC center

110

Neutron ScienceCurrent Status of the Versatile Neutron Diffractometer,
iMATERIA

1. Introduction
Ibaraki prefecture, the local government inJapan in the area where the J-PARC sites are located, has decided to build a versatile neutron diffractometer (IBARAKI Materials Design Diffractometer,
iMATERIA [1]) to promote industrial applications forthe neutron beam in J-PARC. iMATERIA is planned
to be a high throughput diffractometer so that materials engineers and scientists could use it like thechemical analytical instruments in their materials
development process.
This diffractometer is designed to look at a
decoupled-poisoned liquid hydrogen moderator(36 mm, off-centered) (BL20), and to have 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 and a small angle
scattering detector bank. The angular coverage ofeach detector bank is also shown in Table 1. The

rotation speeds for the disk-choppers are the samewith a pulse repetition rate of “25 Hz” for the mostapplications (in normal mode). In this case, the diffractometer covers 0.18 < d (Å) < 2.5 with Δd/d =0.16% at the high resolution bank (BS bank) andcovers 2.5 < d (Å) < 800 at three detector banks of
90 degree, low angle and small angle while gradually changing resolution. When the speed for the
wavelength selection disk-choppers is reduced to“12.5 Hz ”(in wide-d mode), we can access a wider
d-range, 0.18 < d (Å) < 5 with Δd/d = 0.16%, and 5 <d (Å) < 800 while gradually changing resolution.
2. Current status
The three banks, high resolution bank (BS bank),
special environment bank (90 degree bank) and
low angle bank, are operational and the small angle
bank is under commissioning. It takes about 10 minutes (“25 Hz” in normal mode) to obtain a ‘Rietveldquality’ data in high resolution bank at “300 kW” beam
power for about “1 g” of standard oxide samples.

Table 1.	Instrumental parameters of iMATERIA. L2 is thescattered flight path. The d-range for each bank is
the maximum value for the 2-measurement mode.

L1
Guide length
Position of disk choppers

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

High
Resolution
Bank
SpecialEnvironment
Bank
Low
Angle
Bank
Small
Angle
Bank

2θ
L2
d-range2θ
L2d-range2θ
L2d-range2θ
L2d-range26.5 mTotal 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(A°) ≤ 5.0°
80° ≤ 2θ ≤ 100°
1.5 m
0.127 ≤ d(A°) ≤ 7.2
10° ≤ 2θ ≤ 40°
1.2 - 4.5 m
0.37 ≤ d(A°) ≤ 58
0.7° ≤ 2θ ≤ 5°
4.5 m
1.69 ≤ d(A°) ≤ 800

Neutron Science111

3. Automatic sample changer
The automatic sample changer is the most important sample environment for high throughput
experiments. Our automatic sample changer [2]consists of sample storage, two lines of an elevating system, two sets of pre-vacuum chambers anda sample sorting system. We can handle morethan 600 samples continuously at room temperature without breaking the vacuum of the sample
chamber. This year, we modified the drive systemof the automatic sample changer. As a result, measurements speed increased. The sample exchange
time was shortened from 5 to 2 minutes in thismodification.

4. Small sample measurements
Since the beam power increased, it is possible
to measure small-quantity (mg) samples and samples containing large neutron absorption elements
for about one day of beam-time. Fig. 2 shows the
Rietveld fitting pattern of “25.4 mg” YBa2Cu3Oy sample for “18.5 h” at “300 kW” beam power. The goodfitting in Fig. 2 is supported that the neutron diffraction experiment with mg sample can be performed.
The occupation parameter for deficient oxygen site
are 0.910(7) (1b site) and 0.067(5) (1e site), and it
is almost identical with the result of a “1 g” sample
measurement.

Figure 2.	Rietveld refinment pattern of 25.4 mg YBa2Cu3Oy by high resolution bank of iMATERIA using Z-Rietveld.
The measurement time was 18.5 h at 300 kW.

References[1]	T. Ishigaki et al., Nucl. Instr. Meth. Phys. Res. A
600 (2009) 189–191.

[2]	A. Hoshikawa et al., J. Phys.: Conf. Ser. 251(2010) 012083.

T. Ishigaki1, A. Hoshikwa1, M. Yonemura2,3, Y. Yoshida1, T. Matsukawa1, and T. Kamiyama2,3
Frontier Research Center for Applied Nuclear Sciences, Ibaraki University; 2Neutron Science Section, Materials and Life Science Division,
J-PARC center; 3Insitute of Materials Structure Science, KEK

1

112

Neutron ScienceStatus of the High Intensity Total Diffractometer(BL21, NOVA)

1.	In-situ measurement of the hydrogen absorption process of Pd under high-pressure gas
atmosphere
In-situ H2/D2 gas atmosphere measurement isimportant to understand the mechanism of hydrogen absorption and desorption process in materials, since hydrogen contents of hydrogen storage
materials is controlled by the temperature and thehydrogen gas pressure.
On NOVA, a sample environment to control
hydrogen composition in a sample by controllingthe sample temperature and the hydrogen pressure has been equipped. This environment is able
to measure the Pressure-Composition isotherm(PCT) curve and the sample environment is called

PCT environment. The highest H2/D2 gas pressureis 10 MPa with controlling the sample temperaturefrom 50 K to 473 K.
Figure 1 shows PCT curve measured on the
PCT environment of NOVA. A reasonable curve wasobtained. At each deuterium contents, in-situ neutron diffraction measurements were performed andthe observed profiles are shown in Fig. 2. Structuraltransitions from Pd to PdD2 ((1) ~ (4)) and from
PdD2 to Pd ((4) ~ (6)) were observed successfully.
The time-transient measurement of the hydrogen absorption process is shown in Fig. 3. Pd to
PdD2 transition, indicated by the red arrow in Fig. 1,
was measured in about 10 seconds.

5
4
3
2

6
5
4

(2)

(3)

Intensity (a.u.)

(3)

3
2

(2)
(5)

-1

10

6
5
4

(1)

(4)

0

10
Deuterium pressure, P / MPa

Pd-D2 at 393 K

Pd-D2 at 393 K(1.2818 g, 54 mmh, sapphire cell)

(6)

(4)

(5)

(6)

3
2

simulation
Pd

-2

10

6 (1)
5

0.0

PdD

0.2

0.4

0.6

0.8

Deuterium content, D/M
Figure 1.	Pressure-Composition isotherm (PCT) curve of Pd
at 393 K measured on NOVA.

1.0

1.5

2.0
d/Å

2.5

Al2O3

3.0

Figure 2.	In-situ neutron diffraction patterns of Pd during hydrogen absorption and desorption process measured on NOVA. The numbers in parenthesis correspond to the numbers in Fig. 1. The sample cell
was sapphire.

Neutron Science

113

5

Time / sec

Intensity (a.u.)

10of silicon powder. PDF with Vanadium cell for highpressure is almost equivalent with the PDF with
Vanadium cell for ambient pressure, while PDF with
Sapphire cell shows very low real space resolution.
Further improvements of the high-pressure cell andbackground reductions are underway.

20

111
200

1.8

2.0

d/Å

2.2

Pressure V cellRw 13.0%0simulation
Pd
PdD

Si

0

Al2O3

2.4

-20
5

Figure 3.	Time-transient measurement of the hydrogen absorption process of Pd.

Sapphire cellRw 12.3%G(r)0

2.	Improvements of the sample cell for in-situ
measurement under high-pressure gas atmosphere
For total scattering measurement, higher Signalto-Noise ratio should be realized to obtain higher
real space resolution in pair correlation function.
Selection of a sample cell valid under 10 MPa is
one of the keys. At first, the cell had been made withsingle sapphire but it does not display trivial Bragg
spots at higher Q range above 10 Å-1. Alternatively,
vanadium was chosen and used successfully tomake a cell for the high-pressure gas experiment.
Figure 4 shows the Pair distribution function (PDF)-520

Ambient V cellRw 9.5%

0

-20
5

10
r/Å

15

Figure 4.	
PDF of silicon powder measured in Vanadiumcell for high-pressure (top), Sapphire cell for highpressure (middle), and standard Vanadium cell forambient pressure (bottom).

T. Otomo1,2, K. Ikeda1,2, H. Ohshita1,2, N. Kaneko1,2, T. Seya2, and K. Suzuya1
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK

1

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Neutron Science20

BL22: Construction of Energy-resolved Neutron Imaging
System “RADEN”

1. Introduction
The recent developments in the energy-resolved
neutron imaging technique attract significant interest from the fields of science and industry. The
pulsed neutron beam benefits this technique inmany ways, because it makes it possible to perform precise measurements of energy dependent
phenomena using the TOF method with fine energy resolution, and to use simultaneously neutrons
with a wide energy range - from epithermal to cold
neutrons. In J-PARC, we have been developing thepulsed neutron imaging technique [1] and we are
now constructing a new instrument dedicated to thepulsed neutron imaging experiments fully using thepulsed neutron’s nature.
2. Beam line construction
The energy-resolved neutron imaging system,
named “RADEN”, has two primal roles as a pioneering facility for energy-resolved neutron imaging in
the world to perform Bragg-edge imaging [2], resonance absorption imaging [3], and polarized neutron imaging [4], and as a leading neutron radiography and tomography facility in Japan. Based on
this idea, we determined the detailed design of the
instrument, and started the construction.
During the shutdown period in FY 2013, several
installation tasks were completed. At first, the shielding was built at the beam line of BL22 in the 2nd experimental hall of MLF (Fig. 1). Because this instrument not only uses the largest beam and sample size,
but also transports high-energy neutrons, a massive
shield is needed. Therefore, the shield wall consistsof 4 layers, i.e., B4C included mortar, polyethylene,
steel, and concrete, to form an effective radiation
shield. Next, we replaced the heavy shutter with a
new one with 3 different holes, to enlarge the neutron
beam homogeneously up to 300 mm × 300 mm at the
sample position and change the L / D ratio.
Inside the preposition shield tunnel, several optical devices have been installed (Fig. 2): filters, aFigure 1. External view of the beam line shielding.

rotary collimator, a low speed double disk chopper,a fast shutter, another rotary collimator, and a B4C
slit, from upstream. The first rotary collimator makes
a small pinhole to produce higher L / D ratio up to7500 for high spatial resolution imaging. On theother hand, the second rotary collimator is used tolimit the beam size and to suppress the high-energy
neutron background. Filters, which consist of Cd,
Pb, Bi, and acrylic resin plates, are used to transport only epithermal neutrons or to attenuate gamma rays created at the time of neutron generation
for the resonance absorption imaging experiments.
Later, a T0 chopper is also installed in front of thedisk chopper.
A large sample stage with a load capacity of
1.0 ton has been set up in the experimental room
(Fig. 3). This stage has three linear motion axes for
precise sample positioning, and a rotation table sitson the top of the stage. In addition, a small sample
stage was prepared for the CT experiments. Flighttubes filled with He gas, a polarization analysis apparatus, and sample chambers will be installed nextyear.

Neutron Science115

Figure 2. Optical devices inside the preposition shield tunnel.

Figure 3. Photograph of experimental room.

3. Schedule
The rest of construction work will be completed
in FY 2014, including both the counting type andcamera type neutron imaging detectors and computational environment for data analysis. The firstbeam will be accepted after the summer shut downof 2014, and we will start the commissioning study
after that.

References[1]	Y. Kiyanagi et al., Nucl. Inst. Meth. Physics
Research, A 651 (2011) 16.
[2]	H. Sato et al., J. Phys.: Conf. Ser. 251 (2010)
012070.
[3]	K. Kaneko et al., J. Phys. Chem. Solids, 60(1999) 1499.
[4]	T. Shinohara et al., Nucl. Inst. Meth. Physics
Research, A 651 (2011) 121.

T. Shinohara1, T. Kai1, K. Oikawa1, M. Ooi1, M. Harada1, K. Sakai1, T. Nakatani1, M. Segawa2, H. Iikura3, H. Hayashida4,
J. Parker 4, Y. Matsumoto4, S. Zhang4, T. Kamiyama5, H. Sato5, H. Yokota6, T. Sera7, Y. Saito8, K. Mochiki9, M. Kureta2,
K. Aizawa1, M. Arai1, and Y. Kiyanagi10
1
Materials and Life Science Division, J-PARC center; 2NSED, JAEA; 3QuBS, JAEA; 4Neutron R&D Division CROSS-Tokai; 5Hokkaido
University; 6RIKEN; 7Kyushu University; 8KURRI; 9Tokyo City University; 10Nagoya University

116

Neutron ScienceRecent Progress on Polarized Inelastic Neutron Spectrometer
POLANO

1. Introduction
Although the polarized neutron technique has
been developed and used for many years, the application of the time-of-flight (TOF) method has
only been realized in recent years. In particular,
with regard to the inelastic spectrometer, the polarized neutron technique finds limited practical use
in wide scattering angle instruments. In the lightof recent discoveries in material science, many of
the observed complex phenomena are largely due
to the entangled physical degrees of freedom ofspins, charges, orbitals, and even lattice vibration.
In neutron scattering experiments, the varying dependence of momentum, energy, and temperature
can be interpreted by these of degrees of freedoms.
However, a unique, effective, and direct way to observe these properties separately is via the polarization analysis.
The polarization analysis neutron spectrometer
POLANO enables polarization analysis of inelastic
scattering experiments to investigate the dynamical
properties of the above mentioned multiple degrees
of freedom. POLANO is a collaborative project between KEK and Tohoku University under the aegis
of KEK Inter-University Research Program. The
project has been launched in 2009 starting as an
S-type project with financial support from the KENS
neutron facility. After the budget for the project was
successfully sanctioned and obtained, the actual
construction started in 2013. Although part of the instrumental design is still under discussion, the mainconceptual design and manufacturing of the main
components are expected to be completed by theend of 2014.
2. Design & Construction
The spectrometer concepts have compact design with reasonably wide sample space, higher
neutron flux, higher neutron energy polarization
up to 100 meV, and medium resolution. In order to achieve these concepts, the geometrical

specifications of the spectrometer were chosen as
follows, moderator-sample distance L1 = 17.5 m,
sample-detector distance L2 = 2.0 m, and Fermi
chopper-sample distance L3 = 1.85 m.
The shielding design was evaluated based on
gamma and neutron ray tracing by using the Monte
Carlo PHITS code. The POLANO is viewing a decoupled moderator, and the view of the moderator
is 10 cm square in dimension. A radiation dosage ofless than 6.25 µSv/h of surface dose was achieved
with concrete, steel and boric acid as shielding materials. In certain parts of the shielding in the vicinityof the sample space, stainless steel was used as a
non-magnetic material in order to make possible theconduction of high-magnetic field experiments.
To maximize the beam flux at the sample position, focusing supermirror guide tubes with m = 4
have been installed as reported in Ref. [1, 2]. The
use of an elliptical guide tube provides a flux thatis 10 times higher even for 100 meV of neutronenergy. Since the focusing guide tubes affect thebeam divergence, we estimate the beam profile aswell. Figure 1 shows the intensity distribution at L =16.435 m from the moderator, where a SEOP 3He
filter cell will be placed. The beam width at the 3He
filter has a full width of 8 cm at the bottom, and 4 cm
at the half height. In the early stage, 3He cells witha diameter of 5 cm will be used because the 3He
polarizing technique has already been establishedfor 5 cm cells. Since cells with a diameter of 10 cm
have now been developed, the beam exiting thepolarizer will be almost fully polarized in the final
stage. The details on spin polarization in POLANO
and devices are reported in another article [3].
A vacuum chamber is to be installed at the sample-detector section to avoid air scattering and toensure evacuated insulation for the refrigerator. To
ensure flexible use of the sample space, the chamber is designed to be detachable, and is composedof three parts. In addition, B4C vanes and liners areplanned to be installed in the chamber [4]. At the end

Neutron Science117Figure 1.	(a) Evaluated neutron intensity distribution at the 3He cell position. (b) 1D plot of the distribution at
Y = 0. (Ref. [9])of the scattering chamber, position sensitive detectors (PSDs) are to be installed on the inside of thechamber. For energy range of the POLANO, largepressure of 3He gas is not required to achieve reasonable detector efficiency. Therefore, we adopted
the use of a 10 atm gas pressure PSD with 600 mm
effective length and 3/4” diameter. An efficiency of
about 70% is expected for 100 meV neutrons. The
PSDs are arranged in three layers in the vacuum
chamber. The horizontal scattering angle (detector
angle) ranges from −30° to 130°, and the range is±25° along the vertical direction. At first, only horizontal (center) layers are to be fully installed for polarization analysis experiments.
The polarizer, analyzer, and other magnetic devices installed in the POLANO are currently underdevelopment [5,6]. As of the polarizer, a cylindrical3
He spin filter (HeSF) based on the spin-exchange
optical pumping (SEOP) technique will be used topolarize neutrons in the wide energy range. In thesecond stage, a banana-shaped HeSF will be installed as a spin analyzer to study neutrons in the
100 meV region. The large solid angle HeSF will be
installed at a position close to the sample and will
be used in the off-laser mode; consequently, the polarization will undergo decay.
One of the most essential devices for this typeof instrument is the chopper. We have developed
several types of choppers originally for the high118

Neutron Science

resolution chopper spectrometer HRC in the MLF[7, 8]. POLANO will basically use T0 and Fermi
choppers with the same specifications as those of
the HRC. In addition, we plan to use slow rotating
disk choppers (band chopper) and a fast rotating disk
chopper (correlation chopper) to achieve cross-correlation. The T0 chopper is known as a device thatmechanically reduces the intensity of prompt gamma
rays and fast neutrons. For POLANO a T0 chopperwith a frequency of f = 100 Hz of Inconel X750 bladeis adopted for the parameters of beam window widthof w = 80 mm, width of the blade w + 2∆w = 82 mm,
length of the blade (along neutron beam direction) l =300 mm, and radius of the blade R = 300 mm.
At 500 meV of energy (2000 µs of TOF) the background is reduced by nearly 1/100 of that of the incoming beam, and thus the chopper’s performancecan be considered satisfactory. Figure 2 shows thephotograph of a manufactured Fermi chopper thatis similar to the one developed for the HRC. The
following are the design parameters: slit width w =1.2 mm, slot (absorber) width d = 0.3 mm, and rotor
diameter D = 98 mm. A boron-epoxy composite isused for the neutron absorbers in the slit packageof the rotor. The maximum rotational frequency fmax
= 600 Hz is controlled by 25 Hz steps as it tunes
with the proton pulse repetition. The phase can becontrolled fairly precisely; we achieved a phase accuracy of less than 0.3 µs at 600 Hz.

spectrometer for neutron polarization analysis has
begun. The design of most instruments has been
completed, and the main components are to be installed by the end of 2014. R&D of certain devices,
particularly the polarization and magnetic devices
still needs to be performed. In 2015, we plan to carryout radiological assessments. The neutron beams
for the POLANO are expected to be operational in
the beginning of 2015.

Figure 2.	Newly assembled Fermi chopper for POLANO.
(Ref. [9])Two band choppers will be placed along thebeamline to avoid frame overlap. This type of chopper is a single disk chopper made of aluminum coated with boron enriched B4C with epoxy resin. Twodisks rotate at 25 Hz with different opening angles
to select the required channels. A fast rotating disk
chopper is used to achieve cross correlation.
3. Summary
In summary, the construction of the POLANO

References[1]	T. Yokoo et al., J. Phys. Soc. Jpn. 82, SA035(2013).
[2]	T. Yokoo et al., J. Phys. Conf. Series 502,
012046 (2014).
[3]	K. Ohoyama et al., this issue.
[4]	T. Yokoo et al., Review of Scientific Instruments
82, 095109 (2011).
[5]	K. Ohoyama et al., J. Phys. Soc. Jpn. 82,
SA036 (2013).
[6]	K. Ohoyama et al., J. Phys. Conf. Series 502,
012051 (2014).
[7]	S. Itoh et al., Nucl. Instrum. Meth. A 661, 86(2012).
[8]	S. Itoh et al., Nucl. Instrum. Meth. A 661, 58(2012).
[9]	T. Yokoo et al., EPJ Web of Conferences, to be
published.

T. Yokoo1,2, K. Ohoyama3,4, S. Itoh1,2, K. Iwasa5, N. Kaneko1,2, J. Suzuki6, M. Ohkawara3, K. Aizawa7, S. Tasaki8, T. Ino1,2,
K. Taketani1,2, S. Ishimoto2, M. Takeda1,9, T. Oku7, H. Kira10, K. Hayashi3, H. Kimura11, and T. J. Sato11
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Institute of Materials Structure Science, KEK; 3IMR, Tohoku
University; 4WPI-AIMR, Tohoku University; 5Department of Physics, Tohoku University; 6MEC, KEK; 7Technology Development Section,
Materials and Life Science Division, J-PARC Center; 8Department of Engineering, Kyoto University; 9Quantum Beam Science Center, JAEA;
10
Neutron R&D Division, CROSS-Tokai; 11IMRAM, Tohoku University

Neutron Science

119Performance of Spin Devices for Polarized Neutrons of
POLANO

2. Polarizer
POLANO will have a cylindrical 3He spin filter(HeSF) using the on-beam spin exchange opticalpumping method (SEOP) as a polarizer because
Ei = 100 meV is necessary to cover a higher Q region up to 10 Å-1. 3He polarization, PHe, of 72% has
already been realized in Japan [4]. We will use a
GE180 glass cell with a diameter of 3 ~ 5 cm in thefirst stage of the POLANO project. For a future project, HeSF cells with a diameter of 10 cm are alreadybeing prepared at Tohoku University. The polarization tests of the 10 cm cell are already in progress
in JAEA in 2014FY.
An adiabatic fast passage (AFP) NMR will be
installed on the SEOP system because AFP-NMR
can be used as a spin flipper; this is important to reduce the distance between the Fermi chopper andthe sample position, L3.
3. Analyzer
The choice of polarization analyzers for POLANO
is an important technical decision. In the first stage,

120

Neutron Science

we will focus on polarization analysis in Ef < 30 meV;thus, we will install a fan-shaped analyzer with
5.5Qc Fe / Si supermirror benders, similar to thoseused on HYSPEC in SNS and FOCUS in PSI. The
parameters of the bender analyzer of POLANO aresummarized in Table1. The fan-shaped analyzer
bender of POLANO consists of 260 mirrors, which
will be installed by the end of 2014FY; the analyzer
can cover 2θ of about 15~18°. The analyzer will be
set on a table, which rotates around the sample inthe vacuum chamber, thus, users can choose a 2θposition for the experiments. The magnet housing
has an open angle of 40° so that future addition ofsupermirrors will be possible to cover wider scattering angles. For the next stage, banana-shape HeSF
cells are under development.
The transmission of one slit of mirrors is estimated as 0.17 at E = 20 meV under the alignmentof POLANO using McStas, which is consistent withthe data from the supplier company. Figure 1 shows
calculated scattering intensity counted at a pixel ona detector (2 × 2 cm2) from a vanadium pipe withan outer diameter of 25 mm and inner diameter of
24 mm through the fan-shaped analyzer bender.

Int eg Int . [ n/ sec / 2 * 2 c m ^ 2 / 1 MW]

1. Introduction
The polarization analysis technique is quite important in materials science, as it allows us to investigate complicated spin correlations and spin-latticecouplings in magnets, in particular, multipolar orderings in rare earth systems, high-TC superconductors, multiferroic systems and so on.
POLANO, the instrument of this project, will be
the first full polarization analysis spectrometer at
J-PARC [1-3]. KEK has been financially supporting
the POLANO project via the S-type project (2009S09,
2014S09) since 2009. Fortunately, the POLANO
project was funded by a supplementary budget fromthe government in fiscal year 2012 (2012FY), so thefull-scale construction started instantly.
In this article, we report the situations of polarization devices for POLANO and plans for theirdevelopments.

0.20

0.15

400Hz
E=20meV

0.10

0.05

0.00
-1.0

0.0

1.0

Degree [°]Figure 1.	Calculated integrated intensity from a cylindershape vanadium rod counted at a detector (2 ×2 cm2) through a 5.5QC supermirror bender analyzer by McStas. Horizontal axis is the angle of the
optical axis of the supermirror.

Table 1. Parameters of the analyzer supermirror.

MirrorGap
LengthRadius of Curvature
Length of Line-of-Sight

5.5QC (Concave side)
1.5QC (Convex side)
Fe/Si
0.6 mm
258 mm10500 mm
224.7 mm

Substrate
Material
Thicknessborosilicate glass
0.3 mmFigure 2.	Side cross-section of magnetic field distributions
from a solenoid coil for SEOP (left) to a Helmholtz
coil for the sample calculated using ANSYS.

Figure 1 means that the analyzer bender has tobe optimized with accuracy of ±0.2°. The rotation
Table has an optimizing mechanism to satisfy thisrequirement.
4.	Simulation of Distributions of Magnetic Fields
Needless to say, the control of magnetic fields
is the most important factor for successful polarized neutron experiments. We are estimating the
distribution of magnetic fields by the finite element
method using ANSYS software. Figure 2 shows the
distribution of magnetic fields around a solenoid coilfor HeSF and a Helmholtz coil for the sample. Using
the calculated magnetic field data, we could estimate the depolarization along the flight path fromthe SEOP polarizer to the supermirror analyzer
by quantum mechanical treatment. Based on thesimulations, optimized alignments of the magnetic
field devices can be found, which minimizes the
depolarization.
The qualitative estimation of magnetic fields is
indispensable for all the instruments on which polarized neutrons are used. Thus, collaborative discussions about the technical issues have begun in
MLF.

References[1]	K. Ohoyama, T. Yokoo, S. Itoh, J. Suzuki, K.
Iwasa, T.J. Sato, H. Kira, Y. Sakaguchi, T. Ino,
T. Oku, K. Tomiyasu, M. Matsuura, H. Hiraka,
M. Fujita, H. Kimura, T. Sato, J. Suzuki, H. M.
Shimizu, T. Arima, M. Takeda, K. Kaneko, M.
Hino, S. Muto, H. Nojiri, C. H. Lee, J. G. Park,
S. Choi, J. Phys. Soc. Jpn., 82, SA036 (2013).
[2]	
K. Ohoyama, T. Yokoo, S. Itoh, T. Ino, M.
Ohkawara, T. Oku, S. Tasaki, K. Iwasa, T. J. Sato,S Ishimoto, K. Taketani, H. Kira, Y. Sakaguch,
M. Nanbu, H. Hiraka, H. M. Shimizu, M. Takeda,
M. Hino, K. Hayashi, U. Fliges, P. Hautle, J.
Phys.: Conf. Ser., 502, 012051 (2014).
[3]	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, SA035 (2013).
[4]	H. Kira, Y. Sakaguchi, T. Oku, J. Suzuki, M.
Nakamura, M. Arai, K. Kakurai, Y. Endo, Y.
Arimoto, T. Ino, H. M. Shimizu, T. Kamiyama, K.
Tsutsumi, K. Ohoyama, H. Hiraka, K. Yamada,
L. J. Chang, Physica, B 406, 2433 (2011).

K. Ohoyama1,2, T. Yokoo3,4, S. Itoh3,4, K. Iwasa5, M. Ohkawara2, M. Nanbu2, T. Ino3,4, S. Tasaki6, T. Oku3, K. Taketani3,4,and S. Ishimoto4
1
Advanced Institute for Materials Research, Tohoku University; 2Institute for Materials Research, Tohoku University; 3Neutron Science Section,
Materials and Life Science Division, J-PARC Center; 4Institute of Materials Structure Science, KEK; 5Graduate School of Science, Tohoku
University; 6Graduate School of Engineering, Kyoto University

Neutron Science121

Status of Instrumentation for Dynamic Nuclear Polarizationof Proton Spins

1. Introduction
Polarized neutron scattering is a useful method
for studying materials science. A way to polarize
neutron uses a polarized proton target (PPT). As
neutron-proton scattering length of the triplet channel is much smaller than that of the singlet channel[1], the neutron beam transmitted through a PPTgets polarized.
A brute force way to polarize sufficient numberof protons in the target is applying strong external
magnetic field to it and cooling it down to low temperature. However, even if we cool it down to 1 K
and apply external magnetic field of 5 T to it, thethermal equilibrium Boltzmann polarization of the
protons is less than 1% and the target cannot be
used as a practical neutron polarizer.
To highly polarize proton spins, we can use thedynamic nuclear polarization (DNP) method. In theabove mentioned situation, although the polarization of protons is less than 1%, that of unpairedelectrons is nearly equal to unity as the magnetic
moment of electron is much larger than that of proton. The DNP method exploits the microwave-irradiation-driven transfer of polarization from unpairedelectrons to protons. To test the enhancement of the
proton polarization by this method for several target
materials that contain protons and unpaired-electrons and estimate their performance as neutron
polarizers, we are preparing instruments for DNP of
proton spins.
2. Status
To cool a target down and apply external magnetic field to it, we use the cryostat that was usedby Crabb and coworkers [2]. The 4He evaporation
refrigerator can cool the target down to 1 K and thesplit coil superconducting magnet can apply themagnetic field of 5 T to it. Using a ruthenium oxide thermometer and a pressure-gauge for evacuated gaseous helium, we checked the target holder
temperature and found out that it cooled down to122

Neutron Science

1 K. We could also successfully supply a sufficientcurrent for the superconducting magnet to generate
the magnetic field of 5 T.
To measure the enhancement of the proton polarization, we prepared instruments, which are usedin studies of continuous wave nuclear magnetic resonance (CW NMR) spectroscopy. Our system uses
a coil that acts as a transmitter of the radio wavethat is irradiated to the target and a receiver of theradio wave generated by the target material. Whenthe energy difference between the two proton spinstates due to the static magnetic field is equal to thephoton energy of the radio wave generated by thecoil, the radio wave is absorbed and the amplitudeof the reflected voltage from the coil decreases. As
this signal depends on the polarization of the protons and the radio wave frequency [3], we can estimate the polarization enhancement by measuring
the radio wave frequency dependence on the reflected voltages.
To generate the radio wave, we used a frequency synthesizer (Programmed Test Sources
Inc. PTS 250) to apply an oscillating voltage to thecoil. The frequency can be controlled by a digital
signal, which was generated by a digital I/O board(National Instruments, PCI 6509). To measure theamplitude of the reflected voltage from the coil, thehomodyne method was used. The output DC signal was measured by an analog to digital converter(National Instruments, PCI 6281).
To test the CW NMR system, we installed a
Teflon sheet, which contains fluorine nucleus whose
magnetic moment is 6% smaller than that of proton. We scanned the radio wave frequency over therange around the Larmor frequency of fluorine andobserved a clear absorption peak at the expected
frequency as shown in figure 1.
To irradiate a microwave to the target, we prepared
an extended interaction oscillator (Communication& Power Industries, VKT 2438P), which needs water cooling and has a mechanical frequency tuning0.0002

Voltage (V)0.0000− 0.0002− 0.0004− 0.0006− 0.0008
200.1

200.2

200.3

200.4

200.5

200.6

200.7

RadioWaveFrequency (MHz)Figure 1.	Observed NMR spectrum of a Teflon sheet. Thereis an absorption peak with expected frequency.

Figure 2.	Photograph of the extended interaction oscillator,
whose cooling water tubes are removed, the attenuator and the waveguide to transfer the microwave to the cryostat.

system. The center frequency, mechanical tuning
frequency range and typical output power of this oscillator are 140 GHz, 1 GHz and 20 W, respectively.
To optimize the polarization transfer efficiency, we
control the power and frequency of the microwave.
To control the microwave power without changing
the applied voltages to the oscillator, we preparedan attenuator. We also prepared a spectrum analyzer (Agilent, EXA N9010A) and a harmonic mixer(OML Inc., M06HWD) to measure the power andfrequency of the microwave. Figure 2 shows thephotograph of the oscillator, whose cooling watertubes are removed, the attenuator and the waveguide that transfers the microwave to the cryostat.

microwave irradiation, we can estimate the proton
polarization enhanced by the DNP method. Using
this apparatus, we are going to measure the polarization enhancements for several materials whichcontains protons and unpaired electrons, such as
TEMPO(2,2,6,6-tetra-methyl-piperidine-1-oxyl)
doped polyethylene, and estimate their performance as neutron polarizers.

3. Plans
After finishing the setup of the microwave apparatus, we can irradiate a frequency and power
tunable microwave to the target applied 5 T external magnetic field and cooled down to 1 K. By comparing the CW NMR spectrums with and without

Acknowledgement
We thank Yusuke Tochigi for the cooperation in
preparing the CW NMR system.
References[1]	
H. A. Bethe and P. Morrison, Elementary
Nuclear Theory (Wiley, 1956).
[2]	D. G. Crabb, C. B. Higley, A. D. Krisch, R. S.
Raymond, T. Roser, J. A. Stewart, and G. R.
Court, Phys. Rev. Lett. 64, 2627 (1990).
[3]	A. Abragam, The Principles of Nuclear
Magnetism (Oxford University Press, 1961).

K. Taketani1,2, S. Ishimoto3, S. Itoh1,2, K. Iwasa4, K. Ohoyama5,6, S. Suzuki3, and T. Yokoo1,2
Neutron Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3Institute ofParticle and Nuclear Studies, KEK; 4Graduate School of Science, Tohoku University; 5Advanced Institute for Materials Research, Tohoku
University; 6Institute for Materials Research, Tohoku University
1

Neutron Science123Development of a Compact in-situ SEOP 3He Neutron Spin Filter

1. Introduction
We have been developing a 3He neutron spin filter(NSF) for efficient utilization of pulsed neutrons, because the 3He NSF is effective for neutrons in a wide
energy range. The 3He NSF is effective especially forneutrons with energy higher than several-tens-MeV,and can cover a large solid angle and polarize neutrons
without deflecting them from their original trajectory. In
order to apply the 3He NSF to experiments at a pulsed
neutron experimental facility such as the J-PARC, it
is important to make the system compact, stable anduseful. In this study, we have developed a compact insitu spin-exchange optical pumping (SEOP) 3He-NSF
with a spin flip function for the 3He polarization basedon the adiabatic fast passage (AFP) NMR.
2. The instrumental setup
Figure 1(a) shows the instrumental setup of thein-situ SEOP 3He-NSF [1, 2]. The NSF consists of alaser diode, optical lenses and mirrors, and a solenoid coil. A cylindrical glass cell, which contains 3He
gas and a small amount of Rb, is mounted in an oven(Fig. 1(b)). A pickup coil and a radio frequency (RF)coil for the AFP-NMR are mounted around the 3He
cell (Fig. 1(b)) [3]. The oven is placed at the centerof the solenoid. The temperature in the oven is kept
at 450 K to vaporize the Rb while polarizing the 3He
based on the SEOP.

3. Calibration of the AFP-NMR
Pulsed neutron beams transmit through the3
He-NSF, and are counted by a 2-dimensional position sensitive detector (2d-PSD). The intensity ratio R of the transmitted neutrons between a polarized and unpolarized 3He cell is expressed as R =cosh(P3Hesrl), where P3He, s and ρ are the polarization degree, the absorption cross section and thenumber density of 3He. l is the thickness of the 3Hegas. The l is derived from the ratio R0 = exp(-srl)of the neutron transmission with the cell containing
3
He gas and the empty cell. We evaluated the values of l and P3He of three 3He cells by measuring the
R and R0. The obtained values are listed in Table 1.
In order to obtain the relation between P3He and the
NMR signal VNMR, we measured the NMR signal
based on the AFP-NMR method at the same timeas the neutron transmission measurements, anddetermined the ratio Rc = P3He/VNMR.

Table 1. The measured values of l and P3He.

Cylindrical cell size
f34mm × 52mm-L

16.5 atm-cm 0.625

Cell 2f34mm × 52mm-L

10.8 atm-cm 0.436

Cell 3f50mm × 70mm-L

9.6 atm-cm 0.415

(B)

3He

Cell PHe

Pulse neutron
sourceMirror

RF CoilPickup Coil3He cell

Al OvenH䠌

2D-PSND

Al OvenFigure 1. The instrumental setup of the in-situ SEOP 3He-NSF.

Neutron Science(3cmΦ × 5cm l)
RF Coil for
AFP NMR

Solenoid Coil (20cmΦ × 30cm l)

124

P3He

Cell 1(A)
795nm Laser light(Circular Pol.)l

Pickup Coil for
APF and Pulse NMR

4. Spin flip function
By flipping the polarity of the 3He polarization,
the polarity of the generated polarized neutron
beam is alternated. Therefore, a flipping system
for the 3He polarization functions as a neutron spin
flipper. By the AFP-NMR, polarity of the 3He polarization can be p-flipped. In the case of the in-situ
SEOP 3He-NSF, polarity of the circularly-polarizedlaser for the SEOP must be flipped to keep the absolute polarization of the 3He. To change the polarityof the laser, a half-wavelength plate was installed.
The rotation angle of the half-wavelength plate was
optimized, and a polarization of 98% was obtained
for the circularly-polarized laser. The 3He polarization reached 70% and was confirmed to be stablefor over a week.
A demonstration of the 3He-NSF was performedat the neutron reflectometer SHARAKU (BL17).
The in-situ SEOP 3He-NSF was located at 1200 mm
downstream of the sample and used as a neutron
spin analyzer. Cell 2 was used for the 3He-NSF in
this experiment (Table 1). A 2d-PSD was placed after the 3He-NSF. A guide coil was set between thesample and the 3He-NSF for the adiabatic neutron
spin transport.
We performed polarized neutron reflection measurements from a Fe/Cr multilayered thin film withthe giant magneto-resistance effect [4]. By flipping
the spin polarity of incident and reflected neutrons,
we measured the intensity distributions of (+, +),(-, -), (+, -) and (-, +) reflectivities. The first signin the pair indicates spin polarity of incident polarized neutrons and the second that of reflected ones.
Figure 2 shows the reflectivity distributions measured with the applied field of 200 Oe. Off-specularreflections around Qz = 0.08 ­Å-1 were clearly measured in the cases of (+, -) and (-, +). This indicatesthe existence of the antiferromagnetic correlations,which align perpendicular to the applied field direction. The obtained data were well consistent withthe results of Ref. [4].

Figure 2.	
The obtained intensity distributions of the polarized neutron reflectivity from the Fe/Cr thinmulti-layers.

5. Conclusion
We have developed a compact in-situ SEOP
3
He-NSF with a spin flip function for the 3He polarization based on the AFP-NMR. As the relation
between the VNMR and P3He was determined, we
can estimate the P3He by the AFP-NMR. By the
AFP-NMR, polarity of the 3He polarization can be
π-flipped, resulting in the spin flip of the generated
polarized neutrons. The spin flip function for the polarized neutrons was demonstrated by the polarization analysis experiment at the polarized neutronreflectometer SHARAKU (BL17).
References[1]	T. Ino, et al., Physica B, V404 2667-2669(2009).
[2]	K. Sakai, et al., J. Phys.: Conf. Ser. 340, 012037(2012).
[3]	T. Ino, et al., J. Phys.: Conf. Ser. 340, 012006(2012).
[4]	M. Takeda, et al., Physica B, 213&214, 248(1995).

T. Oku1, H. Hayashida1, K. Sakai1, K. Hiroi1, T. Shinohara1, K. Aizawa1, M. Arai1, M. Takeda2, K. Kakurai2, H. Kira3,
N. Miyata3, K. Akutsu3, J. Suzuki3, T. Ino1,4, M. Ohkawara5, and K. Ohyama5
1
Neutron Science Section, Materials and Life Science Division, J-PARC Center; 2Quantum Beam Science Center, JAEA; 3Neutron R&D
Division, CROSS-Tokai; 4Institute of Materials Structure Science, KEK; 5Institute for Material Research, Tohoku University

Neutron Science125

Sample Environment at MLF

1. Introduction
The sample environment (SE) team has been responsible for operating and maintaining of the beamline(BL)-common SE equipment and the development of the SE devices. In FY2013, the SE team
was officially organized in Technology Development
Section in MLF thus succeeding the previous ad hoc
SE team. The newly organized SE team consists ofstaff members from JAEA, KEK and CROSS so as
to be able to support any BL’s across the boundariesof the institutes, no matter if it is a public BL or not.
In this team, we aim at establishing a proper systemcomposed of several professional sub-groups suchas cryogenics and magnets, high temperature, highpressure, soft matter, and so on.
2.	Operation and improvement of the BL-common
SE equipment
At present, a vertical-field superconducting magnet, a 3He-4He dilution refrigerator insert, a high-temperature furnace with a Nb heater and a top-loadingtype 4He cryostat are available or under commissioning as the BL-common SE equipment. In April
2013, we operated the superconducting magnet at
BL18 for its on-beam commissioning (Fig. 1). The
maximum magnetic field of 6.85 T and the lowest
temperature at VTI (Variable Temperature Insert) of

1.17 K were achieved by a single shot mode andkept for more than four hours. Following the operation at BL18, we also operated this magnet at BL14.
The magnetic field was more carefully raised because of an iron frame of its vacuum tank, and thenwe applied the fields up to 4 T without any quenchof the magnet.
For the high-temperature furnace, the accuracyof thermometry was improved. When we used it for
the first time, the location of thermocouples inside
a tube of the sample stick and the short length ofhomogeneous temperature area of the heater element made it impossible to measure the accurate
temperature for a large sample (Fig. 2(a)). We replaced and extended the thermocouples to attach
them directly to the top and bottom of the sample
as shown in Fig. 2(b). Moreover, a control panel for
vacuum pumps and an electric distribution board
were installed for users’ convenience and safety(left panel of Fig. 3). A gas inlet line was equipped(a)thermocouple䠄inside the tube䠅

(b)sample posion

Figure 2.	Sample stick of the Nb furnace, (a) before and (b)after the improvement of the thermocouple position.

Control panel
for vacuum pumps
Electric
distribuon board

Modificaon for experiment
under Ar atmospher
Figure 1. Operation of the superconducting magnet at BL18.

126

Neutron Science

Figure 3. High-temperature furnace after the improvements.

and related modifications made to enable us to conduct a high-temperature experiment under Ar atmosphere. Taking into account the heating up of theouter case of the furnace, we decided on a rule thatan experiment under Ar atmosphere must be performed below 1300°C.
3. Safety measures for top-loading cryostats
In 2012, there was an accident - the center stickof an orange cryostat was suddenly ejected whenchanging the sample due to rapid evaporation of accidentally condensed air inside the sample space.
Responding to this problem, we have taken the following steps to prevent such accidents. We modified the center stick to have an open end and addeda relief valve on the tube just below the top flange
so that the excess pressure is released through theend hole, the relief valve on the center stick andthe original relief valve on the cryostat even when
the bottom of the sample space is sealed by anice block. It is strongly recommended that such a

(a)

(b)

(c)

safety system be introduced in all top-loading cryostats in MLF. As a further step, we applied “D-cuts”
to the baffles. In addition, especially for the insertswith no hollow tubes, such as dilution refrigerator, ashort detachable stainless wire is necessarily connected to the cryostat and its insert when the insert
is pulled up for the sample exchange, to avoid ejection of the insert. Figure 4 shows examples of theapplied safety measures. These modifications arealso recommended for other top-loading cryostats
in MLF.
4. Future plans
A new building for the MLF user support will be
constructed in FY2014. A sample synthesis roomand characterization rooms will be prepared on thefirst floor. We started to discuss the equipment to
be installed there. There will be also a workshop(Fig. 5) for maintenance, long-term commissioning
and modifications of SE equipment and choppers,
whose number has gradually increased, while we
carry out their preparation for user experiments andshort-term commissioning at the SE area in MLF.
Furthermore, we will work on development of the
SE devices at the new workshop. We started to discuss the possible subjects of development for thisfiscal year.

SE and Chopper
workshop(d)䝕䝞䜲䝇ㄪᩚᐊ

Samplesynthesis roomᇶ┙䝉䜽䝅䝵䞁

䜹䝣䜵䝔䝸䜰

Figure 4.	Examples of the applied safety measures; the inserted pictures indicate (a) a relief valve, (b) an
open-end tube, (c) a D-cut baffle and (d) a detachable stainless wire.

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㛤ⓎᐊA

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䠄⏕≀䠅

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ไసᐊ
PSDㄪᩚ

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䝰䝙䝍䞊
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Figure 5.	Sample synthesis room, characterization rooms
and new SE workshop on the first floor of the newbuilding.

T. Aso1, Y. Yamauchi1, Y. Sakaguchi2, K. Munakata2, M. Ishikado2, S. Ohira-Kawamura3, W. Kambara1, S. Takata3,
T. Yokoo3,4, and Y. Kawakita3
1
Technology Development Section, Materials and Life Science Division, J-PARC Center; 2Neutron R&D Division CROSS-Tokai; 3Neutron
Science Section, Materials and Life Science Division, J-PARC Center; 4Institute of Materials Structure Science, KEK

Neutron Science

127

IROHA Upgrade

1. Introduction
We have developed the flexible, scalable andcommon software framework unified data acquisition (DAQ) and device control [1] since the beginning of MLF. The software framework, named“IROHA”, has been introduced and used in several
instruments of MLF since 2008. Last year we started to plan the upgrade of IROHA to achieve higher
flexibility and scalability. We have discussed anddesigned the improvement points in IROHA. The
points of upgrade are specifically as follows.
1)	Proper role-sharing between the device control and the instrument management2)	The interface of the MLF experimental database (MLF EXP-DB) for the management of
measurement information
3)	Platform-independent user interface.
In these articles, we will show the prototype of the
new common software framework for the instrument
control in MLF, named “IROHA2” (shown in Fig. 1).
2.	Roles of the device control server and the instrument management server
In the original IROHA, several device control

servers and the device management server weretightly coupled, which caused difficulty in the maintenance and some problems with the operation. We
redefined the roles of the two servers and clearly
separated these in independent software. The device control server is engaged in each device’s control, such as operation, monitoring and logging of thedevices. The instrument management server, whoserole is the same as the device management serverin the original IROHA, is engaged in the measurement management, including logging of measurements, authorization and certification of users. Each
server is able to run in a stand-alone process as wellas cooperatively. The typical use case is as follows:1)	Calibration of each device by using the device control server in the off-beam2)	Authorization and certification by the instrument management server3)	Configuration of the instrument control system
combined with the DAQ system and the devices.
4)	Calibration of the instrument by using the instrument management server5)	Measurements from the user interface
through the instrument management server.

Figure 1. The schematic diagram of IROHA2.

128

Neutron Science3.	Database interface for the management of
measurement information
The aims of the MLF EXP-DB are to develop acentral management system for experimental data
generated at the facility, and to provide an interface
that gives users’ rapid and effective access to theirown data by using identification information managed in the J-PARC Users Office database. One of
the main roles of IROHA2 is the interface between
the users’ experimental data and the MLF EXP-DB.
When we do a measurement with IROHA2, theinstrument management server collects and records the experimental meta-data, which includes
the conditions of the DAQ system and the devices
as “Run Information” in every measurement. The
MLF EXP-DB automatically searches, registers andcatalogues the Run Information and the experimental raw data, which is read out from the DAQ systemand stored in the disk of the CPU DAQs.
The authorization and certification by the instrument
management server is based on the user information
obtained from the MLF EXP-DB. The instrument management server records the user account in the Run
Information. Using this information, the MLF EXP-DB
recognizes who obtained the experimental data.
4. Platform-independent user interface
At present time, the user interface by means ofa web browser is one of the most platform-independent user interfaces. Particularly, the web pages designed by so-called “Responsive Web” are available
for use from personal computers as well as tablet
terminals and smart phones. We have decided to
introduce the web user interfaces as the new userinterface for IROHA2. We have adopted a framework, BOOTSTRAP [2], to realize the “Responsive
Web” to the user interfaces of the device control
servers and the instrument management server.
Fig. 2 shows the web user interfaces of these servers made by BOOTSTRAP. We can calibrate thedevices, manage the instrument control system anddo a measurement with a web browser.

(a)

(b)

Figure 2.	The web user interfaces of the device control server (a) and the instrument management server (b).

5. Future plan
We will develop several device control servers
for the cryogenic refrigerator, beam narrowers, goniometer and chopper. In addition, the sequence
management server for automatic measurementswith web user interface will be developed. Afterthese developments, we will introduce IROHA2 into
4SEASONS(BL01) in FY2014 and deploy several
instruments in FY2015.
References[1]	T. Nakatani et al., Proceedings of ICALEPCS2009
673-675 (2009).
[2]	http://getbootstrap.com/

T. Nakatani1, Y. Inamura2, and T. Ito3
1
Technology Development Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science Section, Materials and Life Science
Division, J-PARC Center; 3Neutron R&D Division, CROSS-Tokai

Neutron Science

129

A Scintillator-Based Detector with Sub 100-µm Spatial
Resolution for Time-of-Flight Neutron Imaging

1. Introduction
The time-of-flight neutron radiography and neutron tomography are powerful non-destructive techniques for visualizing an object and quantifying theamount of its elementals. However, the specifications
required for neutron imaging place various challenges to the two-dimensional detectors; generally, theseinclude small pixels, a spatial resolution of less than
100 µm, a timing resolution of a few microseconds
and a count rate capability of more than 105 cps.
We have developed a new type of neutron-counting
time-of-flight neutron imager that employs extensively the scintillator and wavelength-shifting (WLS) fiber
technologies. The detector exhibits a high spatial
resolution down to the sub-100-µm level with a low
gamma-ray sensitivity of less than 10−7 at ~ 1 MeV.
2. Scintillator/FOT WLS fiber type detector
Figure 1 shows a schematic view of the neutrondetecting head of the scintillator / Fiber optic taper(FOT) and WLS-fiber detector.
The neutron-detecting head comprises a single
scintillator screen, an FOT, crossed WLS-fibre arrays. The ZnS / 6LiF scintillator absorbs neutrons in a
nuclear reaction of 6Li(n,α)T, and the ZnS scintillator
emits scintillation light. The scintillation light propagates through the FOT while magnifying the light image onto the WLS-fiber arrays. The scintillation image

is magnified, in our case by a factor of 3.1; in otherwords the effective pixel size of the detector becomes
about one-third of the fiber diameter. The WLS fiber
reemits a shifted green light that is transmitted to the
PMTs. The incident position of a neutron is calculatedby the signal processing and encoder electronics
according to the excitation pattern of the PMTs. In
order to achieve the required spatial resolution, thedetector components were carefully selected or developed. Important R&D points were: the thin scintillator screen with thickness of less than 100 µm, theFOT that can perform image magnification with goodlight transmission, and the crossed WLS-fiber arrays
made with the dedicated 100-µm diameter fibers.
Figure 2 shows a photograph of the prototype
detector. The scintillator with thickness of 100 ±10 µm was made in house to match the range ofthe generated triton after the nuclear capture event,which is about 33 µm in the ZnS scintillator. This
scintillator thickness was determined in order toachieve acceptable detector efficiency while minimizing the light dispersion. The WLS-fiber arrays
comprised two fiber ribbons, one in the x and one in
the y direction, each containing 224 fibers. The dyecontent in the fibers was optimized to maximize lightcollection efficiency. The effective diameter of thefiber was 105 ± 7 µm, which included the cumulative error due to the ribbon arrangement. This led to

Detector head

Scinllator/FOT

Figure 1.	A schematic view of a neutron-detecting head of
the prototype detector.

130

Neutron Science

HT distributer

Amp./discri.
cards

Figure 2.	A photograph of the prototype scintillator-based
time-of-flight neutron imager.

the pixel size of the detector to be 34 µm × 34 µm.
The neutron-detecting area was limited to the sizeof the FOT, at 5 mm × 7 mm; this can be increasedby using an FOT with a larger area [1].
Figure 3 provides the example of the measured
beam profiles. Half of the detecting area was covered
with a 1-mm-thick Cd plate, and the measured beamprofile was fitted with the line-spread function. The
mean spatial FWHM resolutions for ten sampled data
points were 80 ± 7 µm and 61 ± 6 µm in the x and y
directions (the mean values for each direction were
derived while excluding the maximum data point).

(a)

4.1

in mm

1.9
Fe
Cu

1 mm

(c)

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㻜㻚㻢

㻜㻚㻠

σ = 29 ± 5 µm

㻜㻚㻞

㻜

㻜

㻜㻚㻝

㻜㻚㻞

13400-13600 µs

Figure 4.	A photograph of a test piece (a), and reconstructed neutron images with a TOF window of 2500–
38000 µs (b), 13000–13200 µs (c) and 13400–
13600 µs (d), respectively. Each image pixel hastime-of-flight information [2].

6SDWLDOUHVROXWLRQ ):+0
= 2.35 σ= 68 ±㻌13 µm

㻜㻚㻤2500-38000 µs(d)13000-13200 µs
㻝

(b)

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Figure 3.	Beam profile with the Cd mask covering the detector face.

3. Demonstration of Bragg-edge-imaging
Figure 4 shows a photograph of a test pieceand reconstructed neutron images with a TOF window measured at BL-10 in the J-PARC/MLF, respectively. The test piece had a cylindrical shape
and was constructed from polycrystalline Cu andFe (Figure 4a). The sample has a length of 6 mm.
The detector was set at 12.7 m from the liquid-hydrogen moderator. In the TOF spectrum the dips
appeared by Bragg reflections of the composite
materials of the sample. The origin of the countdips was clearly identified: one at 13100 µs wasdue to the (110) reflection of Fe, and the other at
13500 µs was due to the (111) reflection of Cu.
The reconstructed neutron images (Figures 4b,c and d) were for times of flight of 2500–38000,
13000–13200 and 13400–13600 µs, respectively.

Figure 4b shows that there was no clear contrast
in the image for a simple transmission measurement. On the other hand, the reconstructed images
in Figure 4c and d contain clear signs of the Cu/Fe
interface. These images demonstrate that the prototype detector produced clear images with fine meshand high contrast by reconstructing the image withthe appropriate TOF window. A separate test with a
60
Co gamma-ray source revealed that the detector
also had a gamma-ray sensitivity of less than 10-7.
4. Summary
We have developed a new type of scintillatorbased time-of-flight neutron imager for energy-selective neutron imaging. The developed detector has apixel size of 34 µm × 34 µm, and the exhibited spatial
FWHM resolution is 80 ± 7 µm and 61 ± 6 µm in the x
and y directions, respectively. The detector also has asuperior 60Co gamma-ray sensitivity of less than 10-7.
References[1]	T. Nakamura et al., 2011 IEEE Nucl. Sci. Sym.
Conference Record, NP1. M-179.
[2]	T. Nakamura et al., Nuclear Inst. and Meth.
Phys. Res., A737 176 (2014).

T. Nakamura1, K. Toh1, T. Kawasaki2, K. Honda1, K. Sakasai1, and K. Soyama1
1
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center; 2Neutron Science Section, Materials and Life Science
Division, J-PARC Center

Neutron Science131

Two-Dimensional Multiwire Neutron Detector with Individual
Line Readout and Optical Signal Transmission

number of events, respectively. The intrinsic spatial
error of the detector is evaluated by fitting the datawith a Gaussian function, and the full width at half
maximum (FWHM) of the spatial error is 1.55 mm.
100
Standard deviation: σ = 76.9
Average gain spread: σ/N = 7.9%

80

Number

A position-sensitive neutron detection system thatconsists of a multiwire-type detector element was developed for the J-PARC/MLF BL17. A photograph ofthe detector head is shown in Figure 1. The sensitive
area is 128 × 128 mm2 with a pitch of 1 mm in both
directions (x and y), and the 256 signal lines are individually readout by signal-processing electronics [1].
The system uses optical devices for a long-distancesignal transmission and insulation between an irradiation area and a data acquisition room.

60
40
20
0

Pressure vessel
Optical fiber

600

800

1000

Counts/pixel

1200

1400

Figure 2.	Histogram of the count distribution of the flat-field
image.

Figure 1. A photograph of the detector head.

Its basic performance was evaluated by an irradiation experiment using a Cf-252 neutron source [2].
The uniformity of all pixels in the two-dimensional
image was ­7.9% as seen in Figure 2. In our detector,
the center of the track of secondary particles, proton
and triton, is defined as the position of the incident
neutron. Therefore, the intrinsic errors are causedby the differences of the track length between protons and tritons. The intrinsic errors are calculated
from the records of all neutron event data and eachtrack length of secondary particles, and plotted in
one-directions in Figure 3. In the figure, the horizontal and vertical axes represent the error and the

Measured signal (counts)

3×104

2×104
1.55 mm FWHM
(0.66 mm σ)

1×104

0

−4

−2

0

Error (mm)2Figure 3. Errors in position detection.

References[1]	H. Yamagishi, K. Toh, T. Nakamura, K. Sakasai
and K. Soyama, J. Instrum. 6 (2011) C12025.
[2]	K. Toh, T. Nakamura, K. Sakasai, K. Soyama
and H. Yamagishi, J. Phys.: Conf. Ser. 528(2014) 012045.

K. Toh1, T. Nakamura1, K. Sakasai1, K. Soyama1, and H. Yamagishi2
1
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center; 2Nippon Advanced Technology, Co. Ltd.

132

Neutron Science4

Study on the In-plane Magnetic Structureof the Neutron Polarizing Multilayer Mirror

1. Introduction
The neutron polarizing supermirrors are someof the most important optical elements to polarize
neutron beams. Soft magnetic properties play a critical role in determining the performance of a polarizing supermirror because it needs to display highpolarization efficiencies at low magnetic fields tomeet a variety of research demands. The magnetic
properties in thin films are known to be improvedby annealing to eliminate stress and to alter the microstructure of the films [1]. This implies the importance of studies on the stress and microstructureof the films. Stress has been proven to be one of
the key parameters for the soft magnetic propertiesof polarizing supermirrors in our previous work [2].
Regarding the microstructure, the magnetic properties of multilayers with polycrystalline grain size lessthan the ferromagnetic exchange length can be explained by the random anisotropy model, i.e. competition between the exchange interaction between
neighboring spins and the local magnetocrystalline
anisotropy [3]. Our purpose is to determine whether
this model is valid in our system by observing the inplane magnetic structure in the magnetization process. Off-specular scattering (OSS) measurementwith polarized neutrons is a unique and powerful
technique to observe the correlations of small magnetic objects in a layered system. This measurement gives access to the in-plane magnetic structure because the lateral correlation length obtainedby the measurement corresponds to the size of anarea with a uniform orientation of the magnetization.
In this study, polarized neutron OSS measurement
was performed for a Fe/Ge multilayer used for polarizing supermirrors.
2. Experimental
Polarized neutron OSS measurement was performed on the BL17 polarized neutron reflectometerwith horizontal scattering geometry installed at theMLF of the J-PARC [4]. A polarized neutron beamwith a wavelength range of 0.2 ≦ λ ≦ 0.8 nm wasavailable in BL17. The resolution in the momentum
transfer in the out-of-plane direction was kept atless than 6.0%. The Fe/Ge multilayer, consisting of
15 bilayers with a bilayer thickness of 20 nm, wasfabricated at JAEA by using an ion-beam sputteringsystem. The external field to the sample was set
to 4.8 × 103 A/m, where the sample was magnetized to 70% of saturation, after being saturated ina field of 8.0 × 105 A/m opposing the guide field of
the neutron beam. This value of the external field
was chosen because the average deviation angle
in areas with a uniform orientation of the magnetization in Fe layers can be considered as 45° sothat the magnetic scattering equally contributes tothe spin-flip and non-spin-flip channels. The data
were collected by a single 3He tube because a 2-D
position sensitive detector was not available in thisbeam time.
The measured OSS images are shown in Fig. 1.
The specular reflection is located at αi − αf = 0, where
αi and αf are the incident and exit angles, respectively. The first, second, and third Bragg peaks areobserved at λ = 0.7, 0.4, and 0.28 nm, respectively.
The scattering arising from the correlation of theinterface roughness is seen in I++ channel whenthe momentum transfer in the out-of-plane direction satisfies the Bragg condition (corresponding to(αi + αf)/λ = const. in Fig. 1). Such scattering is calleda Bragg sheet and means that the interface roughness is correlated in the out-of-plane direction.
Intense magnetic scattering is clearly observed in
I+- and I-+ channels where αi or αi coincides with the
Bragg condition for spin-up state. This is caused by
the large absolute value of the reflected amplitudes
at the Bragg condition (corresponding to λ = 0.68
and (λ − 0.8)/(αi − αf) = 0.57 nm/deg in I+- and I-+
channels, respectively, in Fig. 1). The obtained data
demonstrated that BL17 is suited to measure themagnetic scattering from layered systems.

Neutron Science133Figure 1.	Measured polarized neutron OSS images for Fe/Ge multilayer
consisting of 15 bilayers with a bilayer thickness of 20 nm.

3. Conclusions
Polarized neutron OSS measurement was performed on BL17 for a polycrystalline Fe/Ge multilayer with a grain size less than the ferromagnetic
exchange length to gain insight into the mechanismthat controls the magnetic properties, which are notpresent in the bulk. The magnetic scattering due tothe fluctuated orientation of the magnetization withrespect to the external field was successfully measured. The preparation of a detector covering a wide
range of the scattered angle is definitely needed toincrease the efficiency of the OSS measurement.
The precise data analysis with a simulation basedon the distorted wave Born approximation would

lead to a good understanding of the in-plane magnetic structure of our system.
References[1]	W. Ishiwata, C. Wakabayashi, and T. Matsumoto,IEEE Trans. Magn. 24, 3078 (1998).
[2]	R. Maruyama, D. Yamazaki, S. Okayasu, M.
Takeda, N. Zettsu, M. Nagano, K. Yamamura,
H. Hayashida, and K. Soyama, J. Appl. Phys.
105, 063904 (2012).
[3]	G. Herzer, J. Magn. Mater. 112, 258 (1992).
[4]	M. Takeda, et al., Chinese J. Phys. 50, 161(2012).

R. Maruyama1, D. Yamazaki1, H. Hayashida1, M. Takeda2,3, N. Miyata4, K. Akutsu4, and K. Soyama1
1
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center; 2Quantum Beam Science Center, JAEA; 3Neutron
Science Section, Materials and Life Science Division, J-PARC Center; 4Neutron R&D Division CROSS-Tokai

134

Neutron ScienceScenes from the Neutron Experimental Hall

Genki Tanaka from Kyushu University (left) and Takahito
Yamada from University of Tokyo (right) with a time projection
chamber used for the neutron lifetime measurement at BL05.

Maynard-Casely, Helen preparing the Mito cell for high-pressure neutron experiments at BL11.

Seiko Kawamura (left) and Tatsuya Kikuchi (right) setting thesample stick into a top-loading cryostat at BL14.

Norifumi Yamada checking a sample substrate for neutronreflectivity measurement at BL16 SOFIA.

Takashi Ohhara checking and adjusting the 2-axes goniometer system of the cryostat for BL18, SENJU.

Takuro Kawasaki aligning a sample and optical devices at theEngineering Materials Diffractometer TAKUMI, BL19.

Neutron Science135

Muon ScienceStatus of J-PARC MUSE

The whole J-PARC operation had to be shut
down in May 2013, because of the radioactive
materials leakage incident at the Hadron Hall
Experimental Facility. In this fiscal year, we worked
on proving the reliability of the MUSE facility design
and maintenance, which ensure the target’s safety
against radioactive materials leakage. Finally wemanaged to restart user’s run in February 2014.
1. Reliability of the muon target safety
We have been adopting an edge-cooled non-rotating graphite target, the so-called ‘fixed target,’ because of its ease of handling during maintenance. In
this target, graphite is indirectly cooled by the copper
frame, which surrounds the graphite. This target assembly is equipped with 10 thermocouples. Thoseare incorporated into the interlock system. One is

M1 Line

M1 Lineassigned to be MPS (Machine Protection System),and the other 9 thermometers are designed to alert
the MLF shift leader at the MLF control room. Unlike
the Hadron Facility, at the MUSE facility, we accept
3 GeV protons from RCS with the fast extraction,
but not with the slow extraction. The graphite target
is designed to accept 4 kW of heat deposit at maximum, with an irradiation of 1 MW from the protonbeam, therefore it is not likely to be damaged.
This muon target assembly is contained in thelarge vacuum chamber, in the radiation control area.
Even if the graphite evaporates, any radioactive
contamination is designed to remain in the chamber. Also any exhaust from the chamber throughthe pumping is directed to the MLF stack, which isequipped with HEPA filters and a radiation monitoring system.

S-LineU-LineH-LineD-LineFigure 1.	Six sealing hatches at the boundaries, for the D-Line, U-Line, S-Line, H-Line andtwo M1 beamline exits between M1, M2 tunnels & experimental areas.

138

Muon Science2. Air-circulation
In the M2 tunnel, cooled air by a heat exchanger
are designed to be supplied to the maintenancearea (FL 4–6 m), and retrieved from the ducts under
the M2 floor (FL 0.5 m), in order to prevent damage induced by NOx, and to remove heat by about
5% of Joule heat from the six quadrupole magnets,
four steering magnets, two sets of profile monitor
assemblies, and nuclear reactions. The M2 tunnel
air circulation system, as well as the M1 tunnel air
circulation system, are designed to be circulatingin the closed loop equipped with the pre-filter and
HEPA filter. Therefore, any contamination is designed to be confined in the M1, M2 tunnel, not likely to be leaked into the outside of the control area, if
the boundaries are sealed properly.
3. Sealing at the Boundaries
It is very important to have reliable sealing

between the M1 and M2 areas where radioactive
contamination can be produced by nuclear reactions, and experimental areas where users arebreathing. There are six sealing hatches at theboundaries, for the D-Line, U-Line, S-Line, H-Lineand the two M1 beamline exits between the M1
and M2 tunnels and the experimental areas. The
structure of the sealing hatch is designed to be likedouble layers vacuum flange associated with rubber O-ring, which is shown in the inlets of Fig.1. We
conducted helium leak check by introducing helium
gas into the space between the double layers at
the sealing hatch, which showed 1.2 × 10-7 - 3 ×
10-6 Pa m3/s of the leak rate. It turned out that thesealing hatch was very reliable, including the single
layer’s hatch. On the other hand, the experimental
areas are equipped with HEPA filters and monitoring system to ensure radiation control even in thecase of leakage.

Y. Miyake1,2, N. Kawamura1,2, K. Shimomura1,2, P. Strasser1,2, A. Koda1,2, H. Fujimori1,2, S. Makimura1,2, Y. Kobayashi1,2,
J. Nakamura1,2, K. Nishiyama1,2, Y. Ikedo1,2, K. M. Kojima1,2, R. Kadono1,2, W. Higemoto1,3, and T. U. Ito1,3
1
Muon Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK; 3Advanced Science
Research Center, JAEA

Muon Science139Development of the Muon Production Target at MUSE

A pulsed muon beam with unprecedented intensity will be generated by a 3-GeV 333-microA proton beam on a muon target made of 20-mm thickisotropic graphite (IG-430) at J-PARC/MUSE (Muon
Science Establishment). The energy deposited by a
1-MW proton beam is estimated to be 3.9 kW on themuon target [1]. The first muon beam was successfully generated on September 26th, 2008. Gradually
upgrading the beam intensity, continuous 300-kW
proton beam has been operated since January of2013 [2, 3]. The current muon target with a fixed
target method, called “muon fixed target”, has beenutilized without replacements since the first muon
beam generation. Proton irradiation causes radiation damage to material properties [4, 5]. In particular, the effect to the dimension is significant in ourcase. The proton-irradiation damage of the graphite in the case of the 1-MW proton beam operation
shortens the lifetime of the muon fixed target to lessthan 1 year. Through evaluations of the irradiation
damage, the fixed target was considered to be beyond its lifetime at that time of the scheduled long
shutdown of 2013. To extend the lifetime, the developments of the muon rotating target, in which theradiation damage is distributed to a wider area, hadbeen started since 2008 in parallel with the proton
beam operation [6]. The developments, such as
analyses, detailed designs, and durability tests witha heating and rotating mock-up were completed.
Figure 1 shows the picture of the rotating target.
Figure 2 shows the mock-up of the rotating target.
Safety reviews by relevant experts inside andoutside J-PARC were conducted twice and the reviews validated the installation of the muon rotatingtarget before the long shutdown of 2013. Figure 3
shows a picture taken during the reviews. However,considering the tight schedule and lack of manpower, we determined that we had to extend the time for
installation of the muon rotating target. The muon
rotating target will be installed in the scheduled long
shutdown of 2014.

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Muon Science

Figure 1. Picture of the rotating target.

Figure 2. Picture of the mock-up for the rotating target.

Figure 3. Picture taken during the safety review.

Then, it was re-evaluated whether the use of
the current fixed target could continue. The irradiation effect to the dimensional change of graphite
is proportional to the irradiation dose in the anticipated range for our target. Actually, the rate of thedimensional change depends on the irradiation
temperature. If the irradiation occurs below 570 K,
the graphite will expand. If it occurs over 570 K,
the graphite will shrink. The shrinkage rate is maximized at 1500 K to be 1% per 1 dpa (displacements
per atom). Previously, the maximum shrinkage rate
was applied to the evaluation of the lifetime fromthe point of view of a conservative approach. Then,the beam spot constrained by the un-irradiated surroundings was considered to shrink and crack. Thistime, the rate of the dimensional change dependingon the irradiation temperature is applied to the evaluation. The irradiation temperature depends on the
proton beam intensity, the beam profile on the muontarget, and the thermal conductivities, which also
depend on the irradiation dose. The thermal conductivities, which were actually obtained at MUSE[7], were introduced into the evaluation. As a result,the lifetime was confirmed to be long enough.
The muon fixed or rotating target is rigidly fabricated into the target rod. The target rod is integrated
into the plug shield through four screws, which canbe handled remotely. The assembled components
are called target assembly. Because the muon target is highly activated by proton irradiation, the usedmuon target must be controlled by remote handling.
The used target assembly will be transported by
the shielding vessel, named muon transfer cask,
and stored in the tentative storage pod at the Large
Apparatus Handling Room, which is located at thefloor level of 10 m [8]. Because the rotating target
must stay in vacuum for corrosion control, a storage vessel for the muon rotating target assembly
was installed in December of 2013, in addition toan existent vessel for the muon fixed target assembly. Figure 4 shows a picture of the tentative storage
pod, in which the storage vessels. You can see thevessel for the fixed target on the left and the one forthe rotating target on the right.
After short-term storage, the used target assembly will be transported to the remote handlingroom, i.e. Hot Cell. The used target rod on thetarget assembly is replaced with a new target rod.
The new target assembly, of which the plug shieldis re-used, will be transported to the beam line andinstalled again. For volume reduction of the highly
radioactive components, the used target rod will be
cut remotely into three pieces by the cutting device.
They must be stored in the vessel with a function of
support and enclosure, because they are not selfstanding and radioactive. Because that vessel mustbe transported to another facility for long-term storage, it is called long-term storage vessel. The vessel must be transported by remote control, because
its shielding is insufficient due to weight reduction.
The long-term storage vessel was fabricated andthe planning of the storage scenario was completed. Figure 5 shows a picture of the long-term storage vessel. The commissioning tests in Hot Cell will
be performed from July to September of 2014.

Figure 4.	Picture of the vessels for the fixed and the rotatingtarget in the tentative storage pod.

Figure 5. Picture of the long-term storage vessel.

Muon Science141

References[1]	N. Kawamura et al., Nuclear Instruments andMethods A 600 (2009) 114.
[2]	S. Makimura et al., Proceedings of the 8th
Annual Meeting of Particle Accelerator Societyof Japan, (2011) p1188–1191.
[3]	S. Makimura et al., Nuclear Instruments andMethods in Physics Research A:600 (2009)
146–149.
[4]	T. Maruyama et al., Journal of Nuclear Materials

195 (1992) 44–50.
[5] H. Matsuo, graphite 1991 [150] 290–302.
[6]	S. Makimura et al., KEK Progress Report 20103 M (2010) p6.
[7]	S. Makimura et al., Journal of Nuclear Materials
450 (2014) 110–116.
[8]	S. Makimura et al., Proceedings of the 7th
Annual Meeting of Particle Accelerator Societyof Japan, (2010) p479–483.

S. Makimura1,2, N. Kawamura1,2, S. Onizawa3, Y. Matsuzawa3, M. Tabe4, Y. Kobayashi1,2, R. Shimizu3, Y. Taniguchi1,2,
H. Fujimori1,2, Y. Ikedo1,2, R. Kadono1,2, A. Koda1,2, K. M. Kojima1,2, J. Nakamura1,2, Y. Nakatsugawa1,2, K. Nishiyama1,2,
K. Shimomura1,2, P. Strasser1,2, and Y. Miyake1,2
1Muon Science Section, Materials and Life Science Division, J-PARC center; 2Insitute of Materials Structure Science, KEK; 3Nippon Advanced
Technology Co., LTD (NAT); 4Seekel Co., Ltd.

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Muon Science

Present Status of the D-Line

1. Spectrometer upgrade
The decay muon channel (D-line) of MUSE at
J-PARC delivers 180,000 positive muons per pulse at
the D1 experimental area for the 300 kW operation,
which nowadays is regularly achieved. In order to takeadvantage of this high intensity of the pulsed muon
beam for muon spin relaxation measurement (mSR),
we have developed inexpensive and integrated detector system called Kalliope [1]. Employing 40 unitsof Kalliope detectors installed to a 0.4 T magnet, wehave manufactured a 1280 channel (640 telescopepairs) spectrometer. The spectrometer is installed at
the D1 experimental area as shown in Fig.1.

Figure 1. Full view of the new D1 spectrometer.

The arrangement of the Kalliope units relative tothe magnet is shown in Fig.2. The ethernet hub, theNIM start-pulse distributor as well as the power supply for the Kalliope detectors are placed underneaththe magnet, so that the cables are confined within
the spectrometer.
We started a commissioning of the new spectrometer on February 18th, 2014, the day when the
beam recovered after the Hadron incident. The procedure of the commissioning is (1) determination of
the appropriate bias voltage (HV) for m-APD, threshold DAC (ThDAC) and amplifier DAC (AmpDAC) of
ASIC, and (2) characterization of the mSR spectrasuch as the full asymmetry and the spectrum distortion. The m-APD is provided with a list of minimum
operation voltages distributed within a 0.2 V range
in our spectrometer (66.6–66.8 V). In order to perform (1), we have developed a computer program toscan the DAC values and record a preset number ofaccelerator pulses.
After determining ThDAC for a set of selective combinations of AmpDACs, we took the time
spectrum of the me decay (Fig.3) and tried to findthe appropriate AmpDAC, ThDAC and bias voltages to ensure minimum distortion. Since we received 660k single hits in total for a 100 accelerator
pulse, each counter received ~ 4 positron events(660k/120/1280 = 4.29) per pulse. This high rate of

Figure 2. Diagram of the tail and the side view of the new D1 spectrometer.

Muon Science143

Figure 4.	Forward-backward asymmetry of silver 20 ×
20 mm sample in transverse-field of 2 mT andlongitudinal-field of 10 mT. The data were taken
within 10 minutes with kicker sliced single pulse
operation.

Figure 3.	me-decay spectrum (top panel) and asymmetry(bottom panel) of up-stream counter. Symbols arefor before (triangle) and after (circle) the pile-up
correction.

decay positron signals resulted in a pile-up loss ofcounts in the early stage. We employed a theory ofpile-up correction [2], and found that the simple nonextended correction scheme (eq.(2) of Ref. [2]) was
sufficient to restore the me-decay with the detector
deadtime as an adjustable parameter. The characteristic detector deadtime was estimated to be t ~100 ns for single counters. We phenomenologicallyused the same pile-up correction scheme for coincidenced counts which resulted in a longer deadtimeof t ~ 300 ns. This is because the registered counts
in coincidence are reduced more than the single
counts before coincidence, which determines thecount loss. The deadtime could be improved eventually in electronics, because the recovery tail of them-APD signal is typically ~ 40 ns.
In Fig.4, we show forward-backward asymmetryof a silver sample, after adjusting HV, DACs anddeadtime parameters. The full asymmetry ~ 0.16
is significantly smaller than that of other general
purpose mSR spectrometers (0.2–0.25), because
the positron counters are placed at a high angle(51–60°: see Fig.2) relative to the beam axis, inorder to maximize the detector solid angle while

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Muon Science

accommodating various kinds of inserts. Since
the muon beam intensity is high enough, we plan
to re-position the positron counters to gain higher
asymmetry.
The data acquisition rate of the new spectrometer is 180 Mevents/hour for 20 × 20 mm sample indouble pulse operation, being 4 times higher thanthat of the DΩ-1 spectrometer of J-PARC and/or the
Argus spectrometer of RIKEN-RAL. This high rateof data accumulation requires an automated analysis procedure of mSR measurements, driving thistechnique to a new state of art.
2. Kicker system noise reduction
The muon kicker system is used to separate themuon pulses and feed them to two experimental
areas (D1, D2) simultaneously. The dividing of themuon beam into two single-pulsed beams was successful, but required anti-noise measures. Later, thekicker noise level was drastically improved throughRF-shield with copper sheets and refining both theground lines of the kicker system and the detectors[3].
It turned out that the new spectrometer was influenced by the kicker noise even though in the prototype measures to reduce the kicker noise havebeen taken by refining the ground line of the detector. The new detector, which is an improved version,
has circuit structures more susceptible to noise thanthe prototype.

An outline of the LC circuit is shown in Fig.5. The
noise level of the new detector was ten times higher
when the LC was connected with the power supply A
compared to the power supply B. It was found that thesource was RF noise from the LC itself, which was
propagated through the power cables. The noise disappeared when two bypass capacitors were inserted
between each terminal and the LC housing as shownin Fig.5. It should be noted that grounding to the LC
housing was most effective among other groundings.
Five high-frequency capacitors of 20 nF in parallel were used as bypass capacitors at each terminal
as shown in Fig.6.
Figure 7 shows a comparison between countrates resulting from the kicker noise with and without bypass capacitors. The noise levels were drastically improved after taking the above measures.
In regard to the influence of the kicker noise on
the on-line refrigerator system for the superconducting solenoid magnet, a faulty operation of a bypass valve for thermoregulation in the refrigerator
system caused by the kicker noise occurred during
the beam time. The faulty operation of the bypass

valve resulted in opening the load valve that controls the helium temperature. Fortunately that did
not become a serious matter because the malfunction occurred only once during the day.
The bypass valve is controlled through a VME
bus. Since noises arising from the kicker operation were confirmed at the housing of the VME bus,
the ground line was reinforced with copper seats

(a)

(b)

Figure 7.	Count rates without bypass capacitors (a) andwith bypass capacitors (b).
Figure 5. An outline of the LC circuit.

BypassCapacitors

LC Housing

Figure 6.	Bypass capacitors inserted between each terminal and the LC housing.

Figure 8.	Monitoring system of the on-line refrigerator
system.

Muon Science145to remove the high frequency components in thenoise. Therefore, the noise level at the VME bus
was decreased to about 1/4 as shown in Fig.9.
The urgent measures to reduce the kicker noiseat the New D1-mSR spectrometer and the on-line
refrigerator system succeeded. However, further
improvements are required for negative muons andmuonium experiments at the D2 area. Any conceivable means to reduce RF noises can be employed,
therefore, electrically insulating the kicker chamberfrom the beam ducts and its base and reducing the

ground impedance are considered as a next step.
A kicker system directed the two single-pulsed
muon beams to the two existing experimental areas
D1 and D2 simultaneously in March 2012. Now experiments with the new spectrometer in the D1 area
can be performed with kicker-on without any noiseproblems, but the kicker noise level is still high tocarry out experiments in the D2 area simultaneously. Further measures to reduce the kicker noise arein progress for the next beam operation.

Figure 9. Noise level at the VME bus before/after improvement.

References[1]	K. M. Kojima et al., in KEK-MSL progress reports(2010, 2011 and 2012) and mSR 2014 proceedings, to appear in IOP Conference Series.

[2]	T. Ida, and Y. Iwata, J. Appl. Cryst. 38 (2005)426.
[3]	H. Fujimori et al., KEK-MSL Report 2012 (2013)
16–17.

K. M. Kojima1,2, and H. Fujimori1,2
1Muon Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK

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Muon Science

Present Status of the U-Line

1. Modification and upgrade of the U-line
At the Japan Proton Accelerator ResearchComplex (J-PARC), the second muon beamline,
called U-line, was constructed in the Materials andLife Science Experimental Facility (MLF) [1]. The
main role of the U-line is to provide an intense surface muon source for the ultra-slow muon beam [2].
The ultra-slow muon is an innovative muon beamthat has novel characteristics, such as tunable energy from 0.1 to 60 keV, small beam size, below
5 mm in diameter, and short pulse width of 2 ns,
and is expected to be a new subsurface and interface probe for investigating magnetism.
The installation of the U-line was completed in
the summer of 2012, and the first beam extraction
experiment and beam commissioning were performed right after the installation. These results
have been already described elsewhere [9].
In general, the bulk of contamination in a muon
beam comes from positrons, which have the same
momentum as muons. The positrons are transported with the muon beam and may contribute as
background signals in the detectors for several experiments that we are planning, such as the ultraslow muon microscopy [2] and the g-2 experiment[3]. These positrons will prevent precise measurements, because the yield of positrons in the muon
beam is a hundred times larger than that of muons,according to our simulation of the muon production
process [4]. To avoid this problem, the positrons
in the muon beam must be eliminated completely
before the muons are focused on the experimental target. In order to ensure a wide separation of
the same momentum particles, and also to keep
the trajectories of the muons in a straight line forthe muon transportation after the separator, we selected the Wien filter type separator for the U-line.
The detailed properties and the dimensions of theseparator, and the test for applying high voltage
to the separators have been described elsewhere[9]. We found that it was very difficult to apply highvoltage simultaneously, because of an electricalcorrelation between the separators. This might bedue to some charged particles remaining between
neighboring separators. To avoid this problem, we
decided to change the transportation conditions of
the axial focusing solenoid. We applied high voltage only to the second separator without exciting
the two neighboring solenoids at the front and back,respectively. The transportation and focusing of
the muon beam and positrons in the axial focusing
solenoid were calculated using the Geant4 basedMonte Carlo simulation program, G4beamline [8],and thus confirmed the muon beam transport andthe elimination of the positrons from the muon beam
[9] under these new conditions. Then, we started
the beam commissioning experiments with applying
up to ± 350 kV to the second separator.
We managed to extract high intensity muon beamin the U-line by applying the high voltage only to thesecond separator. To improve the stability of the highvoltage power supply to the separator, i.e. to reducethe discharges in the power supply , we assume thatthe high electric field at the point of the high voltage
power supply is reduced by changing the shape ofthe field relaxing ring of the power supply.
Since the third separator was not used in the
new transport conditions, we decided to replace itwith a fast closing valve (FCV). The FCV is required
to protect researchers in the experimental hall fromradiation exposure caused by unexpected accidents, which may occur in the area of the muon production target. The new design of the axial focusing
solenoid is shown in Fig. 2. The size of the FCV is
320 mm in diameter; it is closed in several tens of a
microsecond when the beamline vacuum worsens
due to an accident. The FCV will be installed in thenext summer shutdown of J-PARC in 2014.
The U-line was installed in the summer of 2012.
The first muon beam extraction experiment was
performed with only the second separator in operation. The result showed that the separator can

Muon Science147eliminate successfully the positrons from the muon
beam. The muon rate was measured by m-e decay
counter and was 6.4 × 107 m+/s. This indicates that
the U-line is currently the highest intensity surface
muon source in the world.
According to the results of the test experiments
for the separator and the beam commissioning, themodifications and upgrades of the U-line, such as
the high voltage power supply of the separator andthe installation of the FCV, are in progress.

Figure 1.	Layout of the muon area in experimental hall No. 2
of MLF/J-PARC.

which are the simplest gas filled radiation detectors
used for detection and quantitative intensity measurements of x-rays, particles and VUV radiations[10]. The gas cell was used at MSL-KEK [11], anda reevaluated one was prepared for the U-line. It
contains parallel plate electrodes that accumulate
nitrogen monoxide molecules ions.
Since the nitrogen oxide gas is toxic, it needs
to be evaluated before using. When the NO gas isoxidized in the air, it converts into NO2 gas. The reaction follows the following chemical formula and athird-order reaction rate equation.
2NO + O2 → 2NO2
The NO2 gas concentration is monitored by the
NO-gas alarm detector. The occupational exposure
limit value is 5 ppm, which should not be exceeded
during any part of the working exposure. 25-ppm
NO2 gas irritates the eyes and the respiratory tract.
Higher concentrations of NO2 gas damage the lungs.
Figure 4 shows a schematic diagram of the piping.
The NO gas is used at the U1 area and a gas station.
The gas station is under the stairs and goes up to the
D cabin. The NO-gas pressure used at the gas cell
is lower than 10 kPa. Even if NO gas leaks from thecell, the concentration is less than 0.3 ppm in a few
minutes at the U1 area, and gradually decreases by
the diffusion and the exhaust. The leak at the U1 area
is considered to be a limited hazard. The worst potential accident would be a leak from a gas cylinder,
which should be prevented with careful attention. In
this case, the NO2 concentration around the cylinder
will increase by more than 103 ppm in a few seconds,
and all the amount of the NO gas will be converted
into NO2 gas in 5 minutes. The concentration of theNO2 gas at the experimental hall 2 is expected to decrease gradually through the air conducting, and become lower than 5 ppm in an hour. It means that theworst accident requires a one-hour evacuation.

Figure 2.	Picture of the muon beam profile at the focal position of the axial focusing solenoid.

2. Laser system
Nitrogen monoxide (NO) gas cell is used formeasuring the intensity of coherent vacuum ultraviolet (VUV) pulsed radiations at the U-line. The concept of the NO gas cell is based on ion chambers,

148

Muon Science

Figure 3.	Schematic drawing of the electric circuit for the NO
gas cell.

Figure 4. Photo of the NO gas cell at the U-line.

The mechanism of the NO gas cell to detect the
VUV radiation is following. The VUV radiation passes through the MgF2 window, which is attached on
an ICF114 flange, and ionizes the NO molecules.
One of the parallel plates accumulates the NO+ in
the NO gas cell. The plate size is 104 mm (wide) ×
50 mm (height), and the distance between plates is
20 mm. The ions rather than the electrons are considered to be collected, because of the photoelectric effect. The absolute intensity of the VUV radiation can be measured by simple analysis, becausea molecule is ionized by one photon. Selective
measurements of the VUV radiation are possible,
because the absorption coefficient of the NO molecules for VUV radiation is larger than that for othercoherent radiations [12]. It means that the NO gas
is transparent for other radiations. Fig. 4 shows theelectric field obtained by simulations of the NO gas
cell with TOSCA / OPERA. The figure at the top left
is the top view of the voltage distribution, and thefigure at the top right is the side view. The figure at
the bottom is an electric field between the window
and the electrode plate. When the gap between thewindow and the electrode plate is shorter, a voltage
drop near the window becomes larger. However,
the electric field is not simply reduced. The efficiency of collection is considered to be dependant on
the electric field. For effective collection of the NO+,
3 mm is adopted for this gap. The 10-mm gap isestimated to create a smaller electric field.
Simple analysis from the measurement voltage
to the intensity of the VUV radiation is following.
After accumulating of the NO+, a 20-nF capacitance

Figure 5. Piping for the NO gas cell.

Figure 6. Electric field calculation of the NO gas cell.

(Fig.1) is charged Q0 quickly. A measured voltage byan oscilloscope (OSC) follows the following formula.
V, C, R, t is a voltage, a capacitance, a resistance,
and a time, respectively. CR = 40 ms is suitable forour 25 Hz pulsed radiation.
V = Q0 / C exp(-t / CR)
If 1-mV high pulse is observed by oscilloscope,
Q0 is
Q0 = V0C = 1 mV × 20 pF = 2.0 × 10-19 C.
The intensity of 122-nm VUV radiation, EV UV
is calculated with a charge of electron Qelectron = 1.6
× 10-19 C, and a photon energy Ephoton = 10.16 eV =980.5 kJ / mol.
EVUV = Q0 / Qelectron × Ephoton = 2:0 × 10-4 mJ
The attenuation of the VUV radiation is also necessary to be considered. The total attenuation by
mirrors and windows is estimated at approximately
0.45.

Muon Science149

References[1] Y. Miyake et al., Physics Procedia 30, 46 (2012)[2]	Y. Miyake et al., AIP Conf. Proc. 1104, 47 (2009)[3] N. Saito et al., AIP Conf. Proc. 1467, 45 (2012).
[4] T. Adachi et al., in preparation.
[5] Y. Ikedo et al., Physics Procedia 30, 34 (2012)[6]	Y. Ikedo et al., Nuc. Inst. and Meth. B, in press(2013)[7]	K. Nakahara et al., Nucl. Inst. and Meth. A 600,
132 (2009).

[8]	Muons, Inc. 522 Nm Batavia Avenue, Batavia,
IL.
[9]	Y. Ikedo et al., in preparation.
[10]	T. Kajiwara et al., Rev. Laser Eng. 12, 367(1984); T. Masuoka et al., Rev. Sci. Instrum. 45,
1012 (1974)[11]	Y. Miyake et al., Nucl. Inst. and Meth. B 95, 265(1995)[12]	K. Watanabe et al., Phys. Rev. 91, 1155 (1953)

Y. Ikedo1,2, and J. Nakamura1,2
1
Muon Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK

150

Muon ScienceConstruction of the S-Line

The construction of the surface muon beamline(S-Line) in experimental hall No.1 of the Materials
and Life science experimental Facility (MLF) building has started. In this fiscal year, the main beamline components to direct the muon beam toward
the S1 experimental area, one of the four plannedexperimental areas, have been manufactured, as
seen in Fig. 1. Three sets of triplet quadrupole magnets SQ7-8-9, SQ10-11-12, and SQ13-14-15 were
fabricated by NEC TOKIN Corp. The basic design ofthe triplet magnets (magnet bore size of f300 mm
in diameter; magnetic pole length of 300 mm) is thesame as that of DQ10-11-12, which was installed in
the D-Line in experimental hall No. 2 by Advanced
Science Research Center, Japan Atomic Energy
Agency (JAEA-ASRC). In addition to this, the magnet support is detachable between the upper andlower parts, in order to facilitate the re-installationin the beamline after alignment. IDX Co., Ltd., refurbished the bending magnet SB2, which had beenpreviously used in the D-Line as DB3. Hitachi, Ltd.,
newly designed and fabricated the septum magnet,
which directs the beam towards the S1 and S2 experimental areas. The details of the septum magnet
together with the new electric kicker system are discussed in another article in this issue [1].

The DC separator (SSEP) was manufactured by
Irie Koken Co., Ltd., designed similarly to the one installed in the D-Line (DSEP); the electrode is 300 mm
in width, 500 mm in length, the gap length is 200 mm,
and the maximum applied high-voltage is ±250 kV,
respectively [2]. However, the HV feed-through wasentirely modified. In the case of DSEP, HV is supplied
through a ceramic insulator. In spite of the designed
value of ±250 kV, the operational voltage is limited
to about ±190 kV because of HV trips. On the other
hand, in the case of the DC separator installed in the
U-Line, the HV stack, which is designed to generate a
HV of ±400 kV by using a Cockcroft-Walton HV circuit,is directly attached to the vacuum chamber [3]. Thisavoids the exposure of the metallic part at HV to theatmospheric environment, thus preventing environment-related HV trips. Therefore, we decided to use
the U-Line style HV power supply (PS) for SSEP. The
HV PS’s were manufactured by NICHICON Corp. withthe same dimensions as those for the U-Line DC separator, so that the PS for the U-Line can be assembled
with SSEP in the case of emergency. It is also notedthat the connecting flange at the vacuum chamber iscommon with that of DSEP. If the PS of SSEP turns
out to be operating successfully, possible upgrade ofPS’s for DSEP might be considered in the near future.

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

Figure 2. Construction of the power supply yard.

Muon Science151

Figure 3.	Installation of the S-Line concrete shields. The
photo was taken without the ceiling shields.

In experimental hall No.1, the construction of thePS yard and the user cabins were completed, together with the plumbing works supplying coolingwater to the PS’s (Fig. 2). The PS yard consists of
3 floors. The upper deck is at 10 m above the floor
level, which is the tallest structure constructed in experimental hall No. 1. The middle deck at the H-Lineexit is connected to the mezzanine at the neutron
experimental area. Nevertheless, emergency stairs
between the upper and middle decks were installed.
It is important to provide more than one evacuationroute in case of emergency.

Shortly after the PS yard was completed, the concrete shields of the beamline were installed, as shownin Fig. 3. The shielding door and the beam stopper in
the S1 experimental area, as well as the beam blocker in the S-Line beamline, were also placed; bothare essential for the MLF operation, even though themuon beam is still not available at the S-Line. On theother hand, the new mSR spectrometer, which will be
installed in the S1 area, as well as the equipment fordata acquisition including the network data storage,
were prepared by Kojima et al. [4].
The construction schedule of the S-Line was not
finalized until the beam operation of MLF started
again in February, 2014, after the long shutdown
due to the radiation trouble at the J-PARC HadronHall in May, 2013. It turned out that the constructionof the beamline by temporary removal of the concrete shields during the beam operation was difficult.
Thus, the beamline components are going to be installed during the shutdown period in FY2014. The
beam commissioning will start in the fall of 2014.
References[1] P. Strasser et al., KEK-MSL Report (this issue).
[2] K. Nishiyama et al., KEK-MSL Report 2009, 7.
[3] K. Nishiyama et al., KEK-MSL Report 2011, 19.
[4]	K. M. Kojima et al., KEK-MSL Report (this issue).

A. Koda1,2, P. Strasser1,2, N. Kawamura1,2, H. Fujimori1,2, K. Nishiyama1,2, and J-PARC Muse staff
1
Muon Science Section, Materials and Life Science Division, J-PARC center; 2Institute of Materials Structure Science, KEK

152

Muon Science

Present Status of the H-Line

A brand new beam line, H-line, is planned to beconstructed as the 4th beam line in MUSE. The newbeam line is designed to have a large acceptance,
momentum tune-ability, and the ability to be used
as a kicker magnet and Wien filter. This beam line
will provide an intense beam for experiments, which
require high statistics and need to occupy the experimental areas for relatively long period. Several
experiments in the field of fundamental physics
studies have been proposed in the H-line [2-4].
From the muon production target, it is possible toextract 4 muon beam lines. The H-line is extracted
to the south east direction.
At the primary stage of MUSE construction, only
the D-line and the frontend magnets in the S-line
were installed, and then the frontend magnets in the
U-line were installed in 2009. In the H-line, temporary radiation-shield blocks were placed. J-PARC
has been operating since 2008, and thus the activation around the muon production target becomes

more serious year by year. According to the evaluation using a Monte-Carlo code [5], the dose rate beside the target chamber was estimated to be close
to 1 Sv/h, and the summer shutdown in 2012 would
be the actual time limit to install the frontend magnets in the H-line. Thus, the installation of the frontend devices, i.e. the muon-capture solenoid, HS1,
the first bending magnet, HB1, and the vacuum
components took precedence and were installed in2012 as shown in Fig. 2 and 3. The measured highest radiation dose rate was about 250 mSv/h in theiron block placed just beside the target chamber.
This is consistent with the prior evaluation. Thus,
the construction scenario based on this estimation
was confirmed to be reasonable.
In the other high intensity beam line in MUSE,
the U-line, we adopted only axial focusing magnets to obtain high transmission efficiency [6]. On
the other hand, in the H-line, the beam captured byan axial focusing large-aperture solenoid magnet

HB1

HGV1

φ600 pillow seal

HS1a

HS1b

Figure 2. Devices installed in 2012.
Figure 1. A layout plan of MUSE.

Muon Science

153

154

Figure 3.	Picture taken on October 4 after completing the
installation of the major devices.

Figure 4.	Final focusing magnet for g-2/EDM; field map (left)
and beam trajectory (right). In this model, a solenoid magnet is examined with a field clump as an
option.

is transmitted through bending magnets, althoughthese non-axial focusing magnets increase thebeam loss. To compensate for this and ensure hightransmission efficiency, large aperture magnets andother devices are adopted in the H-line. A typicalsize of the aperture is 600 mm in diameter.
The magnets and other devices in the downstream are being designed. These devices areplaced in the experimental hall, and thus they have
many design options in sense of material selection, geometrical size and position and so on. In order to provide a satisfactory muon beam to all theplaned experiments in the H-line, designing work is
performed with the collaborations of the proposed
experiments. For instance, the g-2/EDM experiment[3] needs to focus the surface muon beam on themuonium production target, which will be installed
several tens cm apart from the exit of the last magnet. The beam spot size is required to be as small as
possible. In addition, the magnetic field in the muonium production target is required to be smaller than
1 mT, thus the leakage field of the beam line magnet is not negligible in general. Several ideas are
considered for the final focusing magnet. Figure 4
shows a typical result in a case using a solenoid
magnet with a field clump.
The designing work of the radiation shield is alsoin progress similarly to the other beam lines [5]. Alongthe beam line a few meter thick concrete shield will
be necessary to enclose the streaming neutrons andother radiation sources. Because the H-line adopts
large aperture devices, the effects of the streaming
neutrons are more serious than at the other beamlines. The evaluation of the streaming neutrons isimportant not only for the radiation safety but also tocheck its effect on the detectors and other devices
in the experimental area. Figure 5 shows a typicalresult of the simulation. During the time when the
proton beam is on, the dose rate in the experimental
area is expected to exceed 100 mSv/h, and no one
can enter into the area. By inserting a beam blocker
which is a 40-cm thick copper block, the dose rateis decreased by a factor of ten. The beam blocker isessential for the interlock system.

Muon Science(a) blocker out(b) blocker in

100 µSv/h

10 µSv/h

blocker

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

In the summer shutdown in 2014, the radiation
shield between the M2 tunnel and the experimental
hall is planned to be modified and reinforced for the
preparation of the H-line construction in the following year.
References[1]	N. Kawamura et al. 2013 Journal of Physics:

Conference Series 408 012072[2] K. Shimomura et al. ibid.
[3] N. Saito et al. ibid.
[4] S. Mihara et al. ibid.
[5] N. Kawamura et al. 2009 NIM A 600 114.
[6]	K. Nakahara et al. 2010 AIP Conf. Proc. 1222
420.

N. Kawamura1,2, MuHFS collab., DeeMe collab., and g-2/EDM collab.
1
Muon Science Section, Materials and Life Science Division, J-PARC; 2Institute of Materials Structure Science, KEK

Muon Science

155

Scenes from the Muon Experimental Hall

Rotating muon production target to be installed in 2014 is assembled by the target team led by Shunsuke Makimura.

156

Yohei Nakatsugawa and his collaborators assembling a wire chamber which is a proto-type for DeeMe experiment planed in H-line.

A new muon beam profile monitor designed by Takashi Ito is installed
to monitor the beam profile after replacing the spectrometer in D1 area.

A new µSR spectrometer is installed in D1 area by Kenji
Kojima, Masatoshi Hiraishi, Ichihiro Yamauchi, and Hua Li.

Kazuhiko Ninomiya, Makoto Inagaki, Go Yoshida (Osaka Univ.) and
Takahito Osawa (JAEA) installing a new muonic X-ray spectrometerin D2 area toward non-destructive elemental analysis of a meteorite.

Jun Sugiyama, Izumi Umegaki (Toyota central R&D Lab.)and Motonobu Tampo conducting a test experiment for
motion of Li in a battery by detecting muonic X-rays.

Muon Science

Radiation Safety

Radiation Safety

1.	Revision of the J-PARC safety policy after theradiological incident at the Hadron Facility
The radioactive material leak incident occurredat the Hadron Experimental Facility (HD) on May
23, 2013, by accidental incidence of an abnormally
1
short proton beam on the gold target [1] . The gold
target partially melted after being rapidly heated,
and the radioactive products accumulated within
the target were released into the experimental hallsince the air-tightness of the target and the primarybeam line was insufficient.
Because of the incident, the beam operation was
stopped immediately by the interlock system, which
told us that an abnormal beam has been extracted
to the target. In addition, the radiation dose in theexperimental hall gradually increased to 4 µSv/h,
which was definitely higher than usual. However,since such information was not collected and analyzed adequately, nobody could recognize what was
really happening for several hours after the incident.
The staff and the users stayed in the hall after theincident, even though the Hadron Experimental Hall
was entirely contaminated with radioactivity. As a2
result, they received internal exposure .
Furthermore, since the ventilation fans of the hall
were operating, radioactive materials were released
uncontrollably into the environment outside the ra3
diation controlled area .
The applicable laws and regulations say that wehave the responsibility to report immediately radiological incidents to the national authorities and the
local government. Since we misread the scales ofthe personnel exposures and the environmental release of radioactive materials in the early stage, thefirst report to the authorities was delivered at 10 p.m.
on May 24; this means that one and half days had
passed since the primary incident happened.
After we reported the incident, the beam operation of all J-PARC, including the Materials andLife Science Experimental Facility (MLF), had to be
stopped indefinitely.

158

Radiation Safety

In order to resume the operation, we made significant efforts to check the radiation safety of all
facilities other than HD, especially from the view
point of radioactivity confinement capability. In addition, we established a new system for emergency
response to abnormal incidents. Before the HD incident, we had only one status for response to aserious incident, called “Emergency” status. We
learned from the HD incident that we should havean intermediate status for an abnormal incident before it develops into a serious accident; we call it“Alert” status. The conceptual drawing of the structure of the three kinds of risk-management status isshown in Figure 1.
The revision of the J-PARC risk management
plan was reviewed by an external expert panel andreported to the national authority, the local governments and inhabitants in the vicinity of J-PARC. All
staff members and users were introduced to the
new safety framework and emergency drills wereconducted several times. The operation for the MLF
user program could be started on February 17,
42014 . This means that it took 8 months to resume
the beam operation after the HD incident.
In the next chapter we cover in detail what wasdone to restart the MLF operation.

1	At 11:55, due to the malfunction of the power supply
system of a beam extraction magnet of the 50 GeV
synchrotron, 2 × 1013 protons were extracted in 5 msec. (Inthe normal operation 3 × 1013 protons are slowly extracted
over 2 sec.)2	The total number of personnel working in the radiation
controlled area of HD during the incident was 102. As aresult of the measurements with a whole-body counter, it
was found that 34 personnel received detectable internal
exposure in the range of 0.1-1.7 mSv.
3	The “ventilation fun” is just a fan without filtering function
for radioactive material. Ventilation system with filteringfunction had not been equipped in the hadron hall becausethat was assigned as an uncontaminated controlled area.
4	
It will take longer to resume the beam operation of HD
since it will require the target exchange and upgrade of theventilation systems.

Figure 1.	The conceptual structure of the new risk management system of J-PARC. The “Alert” status is newly installed between “Normal” and “Emergency”. In
the “Normal” status, a shift leader makes a declaration of transition to the “Alert” status when aspecified event such as alarm activation from the
Personnel Protection System occurs. In the “Alert”
status, the facility manager or the deputy manage
the status, and they are responsible for collecting information and analysis of the event together
with the facility staff. If they find that the incident isdeveloping or may develop to a real accident, hedeclares transition to the “Emergency” status. (Insome cases such as fire or an undoubtable real
accident, the shift leader has to make the transition directly from “Normal” to “Emergency” status.)
In the “Emergency” status, the emergency headquarters are set up at the Tokai site.

2. Efforts to resume the MLF beam operation
The first thing we had to do to restart the MLF
operation was to recheck the radioactivity-confinement capability of MLF by taking abnormal incidents
into account and to explain the result to the proper
authorities and the external expert panel. The drawing used for explanation of the concept of radioactivity confinement at MLF is shown in Figure 2.
The second thing was to introduce the newrisk-control framework to the MLF management.
Therefore, all operation and user manuals were
fully revised. In addition, the following new manuals
were introduced: shift leader manual, emergency
calling manual, user-evacuation manual and instrument manager manual.
The third thing was training based on the newframework. All MLF staff, including CROSS and
Ibaraki Prefecture staff, participated in the training.
For user training, new video material was produced.

Figure 2.	Conceptual drawing of the multiple protection system for radioactivity confinement of the neutron
target at MLF. The mercury target has a double
wall structure: the mercury container is coveredby the safety hall which has channels of primarycooling water. Therefore, if the mercury container
is ruptured due to pressure wave etc., leakage ofradioactive mercury spills could be prevented. In
addition, the helium vessel and the confinementof the neutron-target station also work as barriers
for radioactivity. On the other hand, the mercury
circulation located in the hot cell is single-barriersystem: the single-barrier just corresponds to thepiping wall of the circulation system, because
there is little possibility for leakage from the piping.
Nevertheless radioactive materials in the hot-cellare always monitored during the proton-beam operation in order to detect a small leak of radioactivity and to take measures to stop leakage as soon
as possible.

The fourth thing was to carry out emergency drills
for radioactive-material leak incidents. The first drill
was carried out on September 13, and the second
one was done on November 15, 2013. The second
drill was positioned as the final test before resuming
the MLF operation, so that the performance was in5
spected by the local governments around the site .
The drill scenario was as follows:●	Radioactive gases are detected by the radioactivity monitor in the hot cell,●	Declaration of transition to “Alert” status by ashift leader,●	Collecting and analysis of radiation monitor dataand other information under the direction of the
MLF manager,

5	The performance of the second drill was reported by alocal TV station and a newspaper.

Radiation Safety159

●	Recognizing the mercury leak from the mercury
circulation system,●	Declaration of transition to “Emergency” status
by the MLF manager,●	User evacuation and radiological survey,●	Taking measures to stop the leakage,●	Reporting to the proper authorities .
3. Radiological license upgrade
Normally we have two chances of the application on radiological license upgrade in a year. This
year, applications on the following items had beenplanned for each chance. In the first application, thefollowing items were to be applied for:a)	Upgrade the proton beam power from 350 keV
to 600 keV,b)	Installation of the slow-muon beam line,c)	Installation of the neutron beam line BL06,d)	Minor changes to the shielding configuration for
preparation of installation of the new neutron

beam lines BL22 and BL23,e)	Setting a radiation controlled area to the extended building hosting BL09.
In the second one, we planned the application on
the following:f)	New installation of the BL22.
However, since the application procedure was delayed seriously due to the HD incident, we had only
one chance in the year and we had to remove theitems (a), (e) and (f) from the application. As a result, we could only apply for (b), (c) and (d). The
application for (a), (e) and (f) was postponed for the
next fiscal year.
Reference[1]	The detailed information on the HD incident canbe found on the J-PARC web site. The addressof the Japanese page is http://j-parc.jp/index.
html and the English page is http://j-parc.jp/
index-e.html.

Y. Kasugai
Neutron Source Section, Materials and Life Science Division, J-PARC Center

160

Radiation Safety

Scenes from the Emergency drill

Masatoshi Arai (Division Head) instructing at the MLF control
room.

Members of the local emergency response headquarters of
JAEA-Tokai site participating in the emergency drill.

Liaison team receiving messages from the JAEA local emergency response headquarters at the MLF control room.

The staff checking the MLF beam status on a display at theMLF control room.

The users evacuating from the MLF experimental hall with theuser evacuation support team.

The users undergoing radiation survey at the MLF entrance
after evacuation from the experimental hall.

Radiation Safety

161Whatʼs new at the MLF in 2013?

Activities of the Technology Development Section

1. Introduction
Activity of the Technology Development Section
started in JFY 2013, which was organized in the
MLF division. This section consists of JAEA andKEK staffs and its tasks are as follows:(1)	Development of common equipment for
beamlines and instruments in the MLF(2)	Operation, maintenance and managementof common equipment for beamlines andinstruments in the MLF(3)	User support of common equipment for
beamlines and instruments in the MLF
In order to perform those tasks, there are four
subgroups in this section, as follows.
(1)	Computer environment subgroup(2)	Radiation and general safety subgroup(3)	Technical support subgroup(4)	Sample environment subgroup
In the view point of unified operation for effective
and safety managements of MLF, the common task
staffs of the Comprehensive Research Organizationfor Science and Society (CROSS) work together
with the Technology Development Section staffs.
Also outsourcing staffs, who work together with subgroups members, are employed for various common tasks.

Figure 1.	Structure of the neutron technology development
section and its relation to CROSS.

164

What’s new at the MLF in 2013?

2. Computer environment subgroup
This subgroup is responsible for the computational environment, data acquisition system anddata analysis software.
The routine works include operation and maintenance of many computers (22 main servers, 3 storages, 3 web computers and 8 database computers, 2 analysis computers, 3 anti-virus computers,
1 system-monitoring computer, 2 backup computers). Experimental data backup, data transfer tostorage, security update, account management,
failure supports of hardware and software, monitoring of storage consumption and network traffic are
included in the works.
A 5-year plan to upgrade the experimental control framework software, IROHA, was fulfilled in thisfiscal year, which added a new function to the instrument management server and device control servers via web-UI stand-alone to the existing IROHA.
A prototype remote-access function, which enables
a user to monitor the experiment, conduct routine
analysis and data download via web is provided andhas been tested by the MLF staffs. Additional remote
access functions dealing with remote login analysis
and simulation for the IROHA upgrade will be introduced, and the experiment database improvement
will be performed according to the 5-year plan. Dataacquisition (DAQ) systems, including scintillator
software, a 3He gas tube and gas electron multiplier(GEM) based detectors have also been in a processof development.
Furthermore, the advanced computing environment for neutron instruments is being designed
now. This environment consists of a high speed
network, large volume storage, management server
and analysis factory. The analysis factory has capability of new computational technique on userfriendly, instant, flexibility and visualization for large
volume data.

3. Radiation and general safety subgroup
This subgroup is responsible for the radiation andgeneral safety and maintenance of common experimental preparation apparatuses. For human safety
and safe operation of the neutron instruments, themembers perform safety examinations of the experimental samples and various kinds of equipment
before the actual experiments. The examination consists of chemical safety check about toxicity, stability
and activation of samples in experimental conditions,as well as mechanical and electric safety check of
the equipment. Sample preparation apparatuses
such as fume hood, glove box and various kinds ofchemical tools are maintained by this subgroup. This
subgroup also evaluates the radiation dose for new
neutron instruments and prepares application forms
for a license to use radiation apparatus.
As a 5-year plan, the deuteration laboratory forthe biological macromolecule and polymer samples,
which is planned at the new user building that will
be opened in next fiscal year have been designedby this group. In the future, the users will be able toprepare complete deuterated samples in the laboratory before the experiment.
4. Technical support subgroup
This subgroup is responsible for the management of the construction schedule of new beamlines
and improvements of various neutron devices. Also
various supports of the neutron instruments’ operation are included in this subgroup. For example,
crane operation for experiment setup and installing new devices, handling and maintenance of mechanical and electric equipment of neutron instruments are also performed by this subgroup. In addition, it deals with the maintenance of the vacuum
pump and various kinds of choppers.

The 5-year plan also envisions the developments of a T0 chopper with 100 Hz rotation speed
and high speed disk chopper with 300 Hz rotation
speed, which will be more stable mechanically andhave longer lifetime than the existing choppers; theassembly of a new Si analyzer for DNA (BL02),
which extends the covered q-ω space, is also being
planned now.
5. Sample environment subgroup
This subgroup is responsible for the maintenance and technical support of common equipment,
and developments of new sample environment apparatus. Standard sample environment apparatuses such as a 7 T superconducting magnet, an Nb
heater furnace and a dilution refrigerator are maintained by this subgroup.
As a 5-year plan, developments of several kindsof advanced sample-environment equipment havebeen started in this fiscal year; they are a pulsed
magnet field system for the strong magnetic field
experiments, a combined system of a low temperature and a high pressure environments for the solidstate physics and the earth science experiments
and a general purpose Pressure-CompositionTemperature (PCT) system for in-situ observationof the behavior of hydrogen absorbing materials.
The development of a compact in-situ SEOPHe spin filter for polarized neutron experiments,
which enables easier setup than the previous prototype, is advancing. Polarization analysis on polarized neutron reflectometry for Fe / Cr multilayers at
SHARAKU (BL17) and separation for the coherent
and incoherent scattering for the silver behenate(CH3(CH2)20COOAg) at TAIKAN (BL15) were successfully carried out.
3

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

What’s new at the MLF in 2013?

165

MLF Operations in 2013

CROSS-Tokai 2013 Update
The Public Neutron Beam Facility at J-PARC
Consistent with its longstanding policy of promoting open access to major publicly-funded research facilities, the Japanese government established in July 2009 the Public Neutron Beam Facility
at J-PARC. The Facility consists of the acceleratorsand target station used to generate pulsed neutron
beams and a proportion of the beamlines that exploit the neutron beams for research purposes.
The legislative framework within which the Public
Neutron Beam Facility was established requires thatan independent third-party organization be responsible for the administration and support of the science program on the so-called ‘Public Beamlines’.
CROSS-Tokai was appointed to this role and began
operations from its offices in the Ibaraki Quantum
Beam Research Center adjacent to the J-PARC sitein early 2011.
Although CROSS-Tokai is structurally independent of JAEA and KEK – the co-owners and operators of J-PARC – it maintains a high level of cooperation and collaboration with the two founding organizations and other stakeholders that is driven byshared scientific objectives.
The Role of CROSS-TokaiCROSS-Tokai is entrusted with specific responsibilities relating to the Public Beamlines which, In

practical terms, can be summarized as follows:	Manage proposal selection and beamtime allocation
	
Provide user support and ancillary experimental facilities
	
Provide assistance and expert advice to existing and potential users
	
Initiate and undertake outreach and facility
utilization promotion activities	Manage the selection and assessment ofContract Beamlines
The Public Beamlines at J-PARC MLF
The MLF has capacity to accommodate up to 23
neutron beamlines around the present target station. There are currently 18 neutron and 2 muon
beam instruments in operation, 1 neutron instrument in commissioning and 3 new beamlines under construction. Of these, 6 beamlines have been
designated as Public Beamlines as part of the
Public Neutron Beam Facility and are supported by
CROSS-Tokai.
Though not exhaustive in their experimental capabilities, the Public Beamlines cover a wide rangeof neutron scattering techniques and can be used ina variety of research fields. The Public Beamlines at
J-PARC MLF are listed in Table 1 with examples of
their research applications.

Figure 1. The Public Neutron Beam Facility at J-PARC (shown in red).

168

MLF Operations in 2013

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

Number

Instrument

Applications

BL01

4SEASONS – 4D-Space Access Neutron Lattice and spin dynamics in condensed matter over a wide
Spectrometer
range of 4D momentum-energy space

BL02

DNA – Biomolecular Dynamics
Spectrometer

Atomic and spin dynamics of biological macromolecules soft
matter and functional biomaterials

BL11

PLANET – High-Pressure Neutron
Diffractometer

Structural analysis and radiography of materials under extreme
pressure and temperature

BL15

TAIKAN – Small and Wide Angle Neutron Nano and micro scale structural analysis of metals, magnetic
Scattering Instrument
materials, soft matter and bio-macromolecules

BL17

SHARAKU – Polarized Neutron
Reflectometer

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

BL18

SENJU – Extreme Environment Single
Crystal Diffractometer

Microcrystalline and magnetic structural analysis of functional
materials

Distribution of Beamtime on the Public Beamlines
The Selection Committee of CROSS-Tokai regularly reviews and sets policies for the distribution of
beamtime on the Public Beamlines at the MLF. In
line with the prescribed role of the Public Beamlines
and taking into account operational requirements,
beamtime is currently distributed in approximately
the following ratios:
CROSS-Tokai in 2013
Overview
After three years of operation, CROSS-Tokai is
now fully engaged in the full range of its mandated
activities: proposal selection via an open and transparent assessment process, provision of high-quality user support, and facility utilization promotion
within both the academic and industrial researchsectors.
At the start of FY2013, CROSS-Tokai was supporting the user program on five fully-operational
Public Beamlines: BL01 4SEASONS, BL02 DNA,

BL15 TAIKAN, BL17 SHARAKU and BL18 SENJU.,
at the same time, BL11 PLANET entered service
as the sixth Public Beamline and was opened togeneral users from the 2013B proposal round. In
addition, construction work continued on the seventh Public Beamline – BL22 RADEN – which will
be available to users in 2015. For information on thecurrent status and science programs on the Public
Beamlines, please see the individual beamline updates in Chapter 3 of this Report.
As the number of Public Beamlines at the MLF
continues to increase, and with strong growth inuser demand for beamtime, CROSS-Tokai has continued to grow as an organization. During FY2013,
the total number of CROSS-Tokai staff rose to 55
with five new team members being employed: all ofthem in the Neutron R&D Division and working in
direct support of the science program on the beamlines.
User operations at J-PARC during the past year,
including those at the MLF, were severely disrupted(a) General Use(d) Director’s Discretion (up to 5%)(b) Elements Strategy Initiative (up to 15%)(e) CROSS-Tokai Research (up to 15%)

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

Facility Use (up to 25%)

Figure 2. Beamtime Distribution on the Public Beamlines.

MLF Operations in 2013169

by the Hadron Incident of May 2013 and its after effects. CROSS-Tokai staff – particularly the beamline
teams – worked furiously with their MLF colleagues
on upgrading safety systems and documentation aspart of the safety audit and strengthening of safety
protocols that was undertaken across the whole
J-PARC site in response to the Hadron Incident.
Ultimately, beamtime for experiments was available
during April-May 2013 and mid-February to the endof March 2014 only. In spite of these challenges, thePublic Beamlines hosted during FY2013, experiments associated with over 100 research proposals
and CROSS-Tokai continued to vigorously promotefacility utilization both in Japan and internationally.
CROSS-Tokai 2013 Highlights
PLANET begins user operations as the 6th Public
Beamline
On 1 April 2013, BL11 PLANET became the sixth
Public Beamline at the MLF and was made available for user operations for the first time in 2013B.
With the addition of PLANET, the range ofscience that can be undertaken on the Public
Beamlines has been extended to include the studyof liquids and solids under conditions of extreme
temperature and pressure using specialist sample
environment apparatus such as the 6-axis multianvil press ATSUHIME.
For more information about PLANET and its capabilities, please see the detailed beamline updatein this report.

Figure 3.	
The ATSUHIME 6-axis multi-anvil press at
BL11 PLANET.

170

MLF Operations in 2013

Trial Use
An important part of CROSS-Tokai’s work inpromoting the utilization of the Public Beamlines is
to grow the user community – particularly amongindustry-based researchers – through outreachand education activities. In addition, from 2012B,
CROSS-Tokai has been operating the Trial Use
Access Program that aims to assist novice users ofneutron-based techniques gain experience and expertise that will allow them to become independent
General Use applicants in the future.
The specific objectives of the Trial Use Access
Program are:		 To grow the user community and,		 	To promote the use and utility of pulsed neutrons through the development and demonstration of innovative new applications
Accordingly, up to a maximum of five percent(5%) of the total beamtime on each of the Public
Beamlines at the MLF can be allocated for Trial Use
experiments in each round.
Employing the specialist expertise and experience of the CROSS-Tokai Science Coordinatorsand other appropriate staff, the Trial Use system offers support to prospective users through the wholeprocess of facility utilization including:		 	Instrument selection and experiment feasibility assessment		 	Proposal preparation		 	Experiment design, planning and execution		 	Data analysis and interpretation		 	Publication of results
The Trial Use program continued to gather paceduring Fy2013 with expressions of interest comingfrom 14 organizations in the industrial and academic sectors. Ultimately, nine projects were developed
into full beamtime proposals and approved by the
Selection Committee. A list of the Trial Use proposals approved in FY2013 is given in Table 2. It is particularly pleasing to note the diversity of science andthe high degree of academia-industry collaborationthat is being encouraged and supported by the Trial
Use program.
We look forward to describing in future reports,scientific outcomes from the Trial use program aswell as the return of Trial use applicants in futurerounds as General Users.

Table 2. Trial Use proposals approved inFY2013.

Round

2013A

2013B

†

Beamline

Applicant organization†

Industry

Research Area

BL02 DNA

Aisin Seiki Co.

Automotive

Polymers

BL15 TAIKAN

Kureha Corporation

Chemicals

Food packaging

BL15 TAIKAN

Taiyo Kagaku Co.

Chemicals

Pharmaceuticals and cosmetics†

BL17 SHARAKU

Asahi Glass Co. .

Inorganic materials

Glasses

BL01 4SEASONSThe University of Tokyo

University

Catalysis

BL02 DNA

Fukuoka University

Automotive

Rechargeable batteries

BL15 TAIKANTOYO Tire & Rubber Co.

Chemicals

Polymer science

BL15 TAIKAN

RIKEN

Govt. Institute

Carbon materials

BL17 SHARAKU

Tohoku University

University

Micro-electromechanical systems

TU experiments approved by the Selection Committee but not carried out due to the Hadron Incident.

Figure 4.	
Food packaging applications of samples studied
in the 2013 Trial Use Program.

Other Key CROSS-Tokai activities FY2013
Proposal Selection	Selection Committee (22 Aug 2013)
		 First meeting of new 2-year term		 	
New Chair (Prof. H. Fukuyama, Tokyo
Univ. of Science) and Deputey Chair(Prof. T. Kanaya, Univ. of Kyoto) elected.
	Public Beamlines proposal selection for 2013B

Proposal Evaluation Committee (16-17 Oct 2013)		 	Call for Proposals (Jun-Jul 2013) – 98
proposals submitted		 	Review by Expert Panels and Proposal
Evaluation Committee (16-17 Oct 2013)		 	Selection Committee (28 Oct 2013) – 30
proposals approved (incl. 5 Trial Use and
1 Proprietary Use)	
Public Beamlines proposal selection for
2014A		 	Call for Proposals (Oct-Nov 2013) – 133
proposals submitted		 	Review by Expert Panels and Proposal
Evaluation Committee (22-24 Jan 2014)		 	Selection Committee (3 Feb 2014) – 74
proposals approved (incl. 4 Trial Use and
2 Proprietary Use)	CROSS Development Proposal Evaluation
Panel (8 Jan 2014) – 3 one-year proposals
approved for FY2014.

Selection Committee (28 Oct 2013)

Figure 5. Public Beamlines proposal selection for 2013B.

MLF Operations in 2013

171

User Support
CROSS-Tokai is now supporting user operations
and ongoing instrument development activities on
the six Public Beamlines with a Neutron R&D teamof 34 scientists, programmers, engineers and technicians. Table 3 shows by type and operation period, the number of research proposals supported
on the Public Beamlines during FY2013.
In addition to our work at the beamlines,

CROSS-Tokai continues to develop and maintainancillary user facilities in the Ibaraki Quantum BeamResearch Center including:		 	User Experiment Preparation Laboratories
I (Sample processing), II (Hard Matter)and III (Soft Matter & Biomaterials).
		 	User Data Analysis Room		 	User Lounge and “Refresh Rooms”

Table 3. Research proposals supported on the Public Beamlines in FY2013.

2013A
2013B

Full year

BL01

BL02

BL11

BL15

BL17

BL18

TOTAL

GU

10

6

-

19

7

8

50

TU

0

1

-

2

1

0

4

GU

3

2

7

6

3

4

25

TU

1

1

0

2

1

0

5

ESI

1

0

0

1

0

0

2

DP

1

1

0

2

0

0

4

PU

3

3

0

6

3

2

17

Instrum.

1

1

1

1

1

1

6

20

15

8

39

16

15

114

TOTAL

GU: General Use				
DP: CROSS Development Proposals†

TU: Trial Use		
PU: JAEA Project Use

ESI: Element Strategy Initiative
Instrum.: Instrument Group Proposals

BL11 was open to GU proposals from 2013B

User Experiment Preparation
Laboratory I

User Experiment Preparation
Laboratory II

User Experiment Preparation
Laboratory III

User Data Analysis RoomUser Lounge

Refresh Rooms

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

172

MLF Operations in 2013

Contract Beamline Review
	Contract Beamline Evaluation Committee		 	16 May 2013 - Finalised procedures, assessment criteria and assessment schedule for the mid-term review of Ibaraki
Prefecture beamlines BL03 iBIX and BL20
iMATERIA.
		 	2 Dec 2013 – Met to discuss the outcomeof review process.
		 	17 Jan 2014 – Finalised review outcome
reports	
The reports prepared by the Contract
Beamline Evaluation Committee were considered by the Selection Committee at the 3
Feb 2014 meeting and CROSS-Tokai advised
Ibaraki Prefecture of the review outcomes on
20 Mar 2014.
Outreach and Facility Promotion
Throughout FY2013, CROSS-Tokai has continued to engage in a wide variety of outreach andfacility utilization promotion activities. Both independently and in collaboration with other stakeholders
in the neutron science community, CROSS-Tokai
convened or otherwise supported in more than 20
events designed to inform new potential users about
the research possibilities of neutrons, disseminate
the latest research results and experimental capabilities and build opportunities for collaboration withother large-scale research facilities.

Highlights of these activities in 2013 included:
	Promotional booths at local and international
conferences	The CROSSroads Workshop Series
	Industrial Applications workshops and user
meetings
	Complementary Use workshops
	Research presentations at local and international scientific meetings

Figure 7.	
The CROSS-Tokai promotional booth at ICNS
(July 2013, Edinburgh UK).

For a comprehensive summary of workshops,
symposiums, seminars, etc. hosted or supported by
CROSS-Tokai in 2013, please see the full listing of
events in Chapter 7 of this report.

MLF Operations in 2013173

Beam Operation Status at MLF
In Japanese Fiscal Year (JFY) 2013, the beam
operation at MLF started with a beam power of
300 kW. Figure 1 shows the trend of the beam power from the first beam to the end of June 2014. For
the accelerator study, a high-power beam of up to
600 kW operated shortly for less than one minute.
In Table 1, the scheduled time and availability
are shown. In JFY2013, we had a good start withhigh availability. Due to the incident at the hadronfacility, the beam operation plan was canceled between May 25 and the end of July so that the availability was very low in Run #49. During the summerof 2013, 400-MeV super conducting LINAC was
installed. After the installation long-duration beamstudies were performed in Run # 50 and 51. The user
beam operation has started in Run #52 on February
18th, 2014, with a beam power of 100 kW due to thevacuum condition at the RCS. The beam operation
with power of 300 kW resumed on February 28th
after degas by the proton beam. During Run #52,
failure events occurred on many occasions at the
LINAC klystron, the LINAC water circulation systemand the RCS shift bump. On average, we had a fairly good availability such as 75%.

600

3000

Table 1. Run cycle, scheduled time and availability.

Run#
48
49
50
51
52
Overall

Scheduled Time (h).
250993
No time for user
No time for user
889
2132

500

2500

400

2000

300

1500

200

1000

100

500

Accumulated power (MWh)Beam power (kW)Beam power
Accumulated beam power002008/5/30 2009/5/30 2010/5/30 2011/5/30 2012/5/30 2013/5/30 2014/5/30

Date

Figure 1.	Beam power trend at MLF and cumulative beam power from the first beam
to the summer of 2014.

174

MLF Operations in 2013

Availability
99.0
58.6

86.2
74.8

Users at the MLF
In fiscal year 2013, there was a long periodof the accelerator shutdown due to an incident in
the Hadron Facility which is one of the facilities in
J-PARC. The resumption of operation was approvedin January 2014. Therefore, the number of neutron
users at the MLF in fiscal year 2013 decreased fromthat in the previous fiscal year, while the number ofmuon users a little bit increased. Since upgrade ofthe linear accelerator is planned, more users thanever are expected to come to the MLF in the next
fiscal year. The transition of the number of users
at the MLF is summarized in Table and Figure fordomestic and foreign users of neutron and muon
experimental facilities.

Table. The number of domestic and foreign users in the period of fiscal year.

FY2008FY2009FY2010FY2011FY2012FY2013

Domestic Foreign Domestic Foreign Domestic Foreign Domestic Foreign Domestic Foreign Domestic Foreign
Users
Users
Users
Users
Users
Users
Users
Users
Users
Users
Users
Users
Neutron
Muon

182
161

378
21

353

12
12

529
25

485

57
0

55

222
44

198

55
2

48

735
24

650

30
7

28

520
85

452

72
2

62

Muon (foreign users)

Neutron (foreign users)

Muon (domestic users)

Neutron (domestic users)

68
77

10

62

15

900
750
600
450
45
300
30
FY 2008

150
15
FY 2009

FY 2
2010
0

2011
FY 201
1

2012
FY 2
012

0
FY 2013

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

MLF Operations in 2013

175

176

MLF Operations in 2013

Muon Program
Advisory Comm.

Muon Science
Proposal Rev. Comm.

Contract Beamlines
Only

Unified
Access Point

Task Forces(CROSS)

Registered
Ins tu on

Proposal
Evalua on Comm.

Public Beamlines Only

ALL Proposals submi ed via the J-PARC Users Office

Neutron Science Proposals

Public Beamlines Only
JAEA Research
CROSS Development
Proposal Advisory Proposal Evalua on
Commi ee
Panel
Joint Meeng

Joint Meeng

Neutron Science
Proposal Rev. Comm.

All except Public
Beamlines

All except Public Beamlines
Neutron Program
Advisory
Commi ee

Neutron Instrument
Proposals

Joint Meeng

Neutron Instrument Contract Beamline
Proposal Rev. Comm. Evalua on Comm.

All except Contract
Beamlines

Selec onCommi eeDirector
CROSS-TokaiMLF Advisory
Board

Collabora on
Commi eePresident
CROSS

Public Beamlines Only

Director
J-PARC

President
JAEA

All except Public Beamlines

Muon Science Proposals

Muon
Instrument
Proposals

Muon Instrument
Proposal Rev. Comm.

(JAEA/KEK)

J-PARC
CenterDirector General
KEK

The JAEA-KEK-CROSS Agreement of Coopera on on the Promo on of Public U liza onof the Specific Neutron Beam Facili es at J-PARC (Enacted on 1 April 2011)

Proposal Review System

MLF Proposals Summary – FY2013
Table 1. Breakdown of Proposal Numbers for the 2013A & 2013B Rounds.
Beamline
BL01

2013A
Submitted
Approved
PU/S IU
GU
PU/S IU
GU

Instrument
4D-Space Access Neutron Spectrometer- 4SEASONS

BL02 Biomolecular Dynamics Spectrometer - DNA
BL03

Ibaraki Biological Crystal
Diffractometer - iBIX

(100-β)

‡

(β)†

2013B
Submitted
Approved
GU
PU/S IU
GU
PU/S IU

12(1+)

3

2

10(1+)

3

2

13(1#, 1+)

3

2

5(1#, 1+)13(1#)

3

2

7(1#)

3

2

10(1#)

3

2

3(1#)

3

2

4

0

0

4

0

0

1

0

0

1

0

0

3

2

0

9

0

0

9

0

0

9

0

0

9

0

Accurate Neutron-Nucleus Reaction
BL04
Measurement Instrument - ANNRI

6

1

1

6

1

1

4

1

1

4

1

1

BL05 Neutron Optics and Physics - NOP

1

1

0

1

1

0

3

1

0

3

1

0

9

1

0

9

1

0

3

1

0

3

1

0

0

1

0

0

1

0

0

1

0

0

1

0

7

2

1

7

2

1

5

2

1

5

2

1

BL11 High-Pressure Neutron Diffractometer - PLANET

0

1

0

0

1

0

7

1

0

7

1

0

BL12 High Resolution Chopper Spectrometer- HRC

2

1

0

2

1

0

2

1

0

2

1

0

11

2

1

11

2

1

6

2

1

6

2

1

27(2#, 1+)

6

3

22(2#, 1+)

6

330(2#, 1+)

6

3

9(2#, 1+)

6

3

15

1

0

15

1

0

7

1

0

7

1

0

#

Super High Resolution Powder Diffractometer
BL08- S-HRPD
Special Environment Neutron Powder
BL09
Diffractometer - SPICA
Neutron Beamline for Observation and
BL10
Research Use - NOBORU

Cold-neutron Disk-chopper Spectrometer
BL14- AMATERAS
Small and Wide Angle Neutron Scattering
BL15
Instrument - TAIKAN
High-Performance Neutron Reflectometer with a
BL16
Horizontal Sample Geometry - SOFIA

#

#

#

BL17 Polarized Neutron Reflectometer - SHARAKU

9(1 )

3

1

9(1 )

3

1

15(1 )

3

1

5(1 )

3

1

Extreme Environment Single Crystal Neutron
BL18
Diffractometer - SENJU

8

2

2

8

2

2

4

2

2

4

2

2

31(1+)

3

1

16(1+)

3

1

5

3

1

5

3

1

6

0

0

6

0

0

3

0

0

3

0

0

(β)†

0

25

0

0

25

0

0

23

0

0

23

0

BL21 High Intensity Total Diffractometer - NOVA

12

1

0

12

1

0

5

1

0

5

1

0

D1

19

1

1

19

1

1

5

1

1

5

1

1

BL19 Engineering Diffractometer - TAKUMI
BL20

Ibaraki Materials Design
Diffractometer - iMATERIA

Muon D1(100-β)‡D2

Muon D2

5

0

1

5

0

1

5

1

0

5

1

0

U

Muon U

0

1

0

0

1

0

0

1

0

0

1

0

79

19

169

68

16

279

76

18

87

67

15

Subtotal
Total

229

327

253

169

373

GU : General Use		
PU : Project Use or Ibaraki Pref. Project Use
IU : Instrument Group Use
S : S-type Proposals† : Ibaraki Pref. Exclusive Use Beamtime (β = 80% in FY2013)‡ : J-PARC Center General Use Beamtime (( 100-β = 20% in FY2013)# : Proposal Numbers under Trial Use Access System in GU+ : Proposal numbers under Element Strategy in GU

MLF Operations in 2013177

Proposals

400
114

300
200
34
67

100
0

124

4
90

33

21

21

16

150

166

159

74

28
12
89

225

235

253

204

Not Approved
Approved

169

2008 2009A 2009B 2010A 2010B 2011A 2011B 2012A 2012B 2013A 2013B
Proposal Round
Figure 1. MLF Proposal Numbers over Time.

Table 2. Principal Investigator Affiliations in FY2013.

Universities(Japan)

JAEA

Companies(Japan)KEK

Foreign
Organizations

Research Institutes(Japan)

289

154

84

40

55

78

ResearchInstute (Japan)
11%
Foreign
Organizaon
8%
KEK
Companies(Japan)
6%
12%

Universies(Japan)
41%
JAEA
22%

Universies(Japan)
JAEA
Companies (Japan)
KEK
Foreign Organizaons
Research Instutes (Japan)

Figure 2. Origin of Proposals in FY2013.

Figure 2 : Origin of Proposals in FY2013

178

MLF Operations in 2013

Table 3. Proposals by Sub-committee/Expert Panel – FY2013.

Sub-committee
Expert PanelQ1

4%
No.
of Proposals
P10
2013A
1%

P8
5%

P9
No. of Proposals
2%
2013B

P2

P3

P4

57

15

21

11

Q2
8%66

16 P1

25%

P7
11%

P6
2%

P8
5%

P1

P9
2%

Q1
4%

P10
1%

P5
21%

P4
5%

Q2
8%

(a) 2013A

P7
11%
P5
21%

P6
2%

35

P3
9%

P1
25%

P4
5%

P3
9%

(a) 2013A

P5

Q2
9%

P7
12%
P6
11%

P1
29%

P2
7%

Q1
5%

P10
P9 1%
2%
P7
12%
P6
11%

Q2
9%

P1

(b) 2013B 29%

P8

P9

P10

Q1

Q2

P1 : Crystallography
5
24
12
4
3
8
18
P2 : Liquid and Amorphous Materials
P3 : Nanomaterials
70
24
27
5
2
11
21
P4 : Biomaterials
P2
P5 : Magnetism and Strongly-Correlated Systems
7%
P6 : Fundamental Physics
P7 : Industrial Applications
P8 : Research and Development
P9
Use
P1 :: Trtial
Crystallography
P10: Element Strategy
P2 : Liquid and Amorphous Materials
Magnetic and Strongly Correlated Electronic Materials
Q1
P3 :: Nanomaterials
Q2
Chemical Physics and General Science
P4 :: Biomaterials
P2
P5 : Magnetism and Strongly-Correlated Systems
7%
P6 : Fundamental Physics
P7 : Industrial Applications
P8 : Research and Development
P9 : Trtial Use
P10 : Element Strategy
Q1 : Magnetic and Strongly Correlated Electronic Materials
Q2 : Chemical Physics and General Science

P3
16%

P5
31%

P7

46

Q1
5%

P10
P9 1%
2%

P6

P2
7%

P1 : Materials Science and Engineering
P2 : Energy ScienceP3 : Soft Matter, Biomaterials and Liquids
P4 : (Reserved)
P5 : Magnetism and Strongly Correlated Electron Systems
P6 : Fundamental Physics, Nuclear Science and Instrument R&D
P7 : Industrial Applications
P8 : (Reserved)
P9
Use Access Program
P1 :: Trial
Materials Science and Engineering
P10: Element Strategy
P2 : Energy Science
Q1
Electronic Properties of Matter
P3 :: Soft
Matter, Biomaterials and Liquids
Q2: Hydrogen in Matter & General Applications
P4 : (Reserved)

P5 : Magnetism and Strongly Correlated Electron Systems
Figure 3. Submitted Proposals by Sub-committee/Expert– FY2013.
Physics,
Nuclear Science and Instrument R&D
P6 : Fundamental Panel

P3
P5
16%
P7 : Industrial Applications
31%
Figure 3 : Submitted Proposals by Sub-committee/Expert Panel – FY2013
P8 : (Reserved)*Subcommittees/Expert Panels were re-structured and re-categorized from 2013B.
P9 : Trial Use Access Program
P10 : Element Strategy
Q1 : Electronic Properties of Matter
Q2 : Hydrogen in Matter & General Applications(b) 2013B

Figure 3 : Submitted Proposals by Sub-committee/Expert Panel – FY2013*Subcommittees/Expert Panels were re-structured and re-categorized from 2013B.
MLF Operations in 2013179

MLF Division Staff 2013
Head		
Deputy Head					

Masatoshi Arai (JAEA)
Hideki Seto (KEK)
Masatoshi Futakawa (JAEA)

Neutron Source Section
JAEA
Hiroshi Takada
Yoshimi Kasugai
Katsuhiro Haga
Shinichiro Meigo
Kenji Sakai
Makoto Teshigawara
Hidetaka Kinoshita
Masahide Harada
Hiroyuki Kogawa
Takashi Wakui
Masakazu Seki
Akihiko Watanabe
Akira Ogawa
Kiichi Ohtsu
Shinji Komori
Kiyomi Ikezaki
Kohei Hanano

Leader
Sub-Leader
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		

		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		

Hideki Tatsumoto
Motoki Ohi
Yoshihiko Kawakami
Hideki Ueno
Tomoyuki Kawasaki
Takashi Naoe
Atsushi Akutsu
Toru Suzuki
Masato Ida
Hideaki Ishii
Shizuka Yoshinari
Chieko Higuchi
Shoichi Hasegawa*Hiroki Matsui*
Tomokazu Aso*
Kenichi Oikawa*
Tetsuya Kai*

Neutron Science Section
Leader
		
		
		
		
		
		
		
		
		
		
		
		
		
		

180

KEK
Takashi Kamiyama
Hideki Seto
Toshiya Otomo
Hitoshi Endo
Tetsuya Yokoo
Norifumi Yamada
Shuki Torii
Kaoru Taketani
Kazutaka Ikeda
Masao Yonemura
Haruhiro Hiraka
Hidetoshi Ohshita
Miki Nagao
Shinichi Ito
Takashi Ino

MLF Operations in 2013

		

Naokatsu Kaneko

Sub-Leader
		
		
		
		
		
		
		
		
		
		
		

JAEA
Yukinobu Kawakita
Kentaro Suzuya
Kenji Nakajima
Ryoichi Kajimoto
Takanori Hattori
Mitsutaka Nakamura
Stefanus Harjo
Nobuaki Takahashi
Takenao Shinohara
Takashi Ohhara
Tetsuya Kai
Kenichi Oikawa

		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		

Seiko Kawamura
Shinichi Takata
Ryoji Kiyanagi
Kaoru Shibata
Takuro Kawasaki
Yasuhiro Inamura
Tatsuya Kikuchi
Taiki Tominaga
Takaaki Iwahashi
Tomonori Hosoya
Kazuhiro Aoyama
Chiho Tobe
Naoko Shimizu
Naoko Kawase
Masayasu Takeda*
Toyotaka Osakabe*Kazuo Kurihara*

		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		

Shuichi Wakimoto*
Itaru Tamura*
Koji Kaneko*
Satoru Fujiwara*
Hiroshi Nakagawa*Asami Sano*
Hidehito Asaoka*
Masato Kubota*
Hideo Harada*
Atsushi Kimura*
Shoji Nakamura*
Yosuke Toh*
Mariko Segawa*
Hiroshi Iikura*
Masahide Harada*
Kazuya Aizawa*
Wataru Kambara*

		
		
		
		
		

Mitsutaka Nakamura*
Nobuaki Takahashi*
Shinichi Takata*
Kaoru Sakasai*
Tatsuya Nakamura*

		
		
		
		
		
		
		
		
		
		
		
		

KEK
Masataka Sakaguchi
Tomohiro Seya
Setsuo Satoh
Tetsuya Yokoo*
Shuki Torii*
Kaoru Taketani*
Takashi Ino*
Naokatsu Kaneko*
Kenji Kojima*
Naritoshi Kawamura*
Hiroshi Fujimori*Shunsuke Makimura*

Technology Development Section
Leader
Sub-Leader
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		

JAEA
Kazuya Aizawa
Takayuki Oku
Tomokazu Aso
Takeshi Nakatani
Wataru Kambara
Hiromichi Tanaka
Yukihiro Ito
Yasuhiro Yamauchi
Shino Ono
Kentaro Moriyama
Wu Gong
Yukino Inoue
Chikako Doda
Yoshimi Kasugai*
Kenji Sakai*
Tetsuya Kai*
Hiroyuki Kogawa*
Motoki Ohi*
Kentaro Suzuya*

MLF Operations in 2013

181

Neutron Instrumentation Section
Leader
		
		
		
		
		

JAEA
Kazuhiko Soyama
Kaoru Sakasai
Dai Yamazaki
Kentaro Toh
Tatsuya Nakamura
Ryuji Maruyama

		
		
		
		
		
		

Hirotoshi Hayashida
Katsunori Honda
Hiroyuki Suzuki
Hideshi Yamagishi
Noriko Amezawa
Takuro Sakai*

Muon Science Section
Leader
		
		
		
		
		
		
		
		
		
		
		
		
		
		

KEK
Yasuhiro Miyake
Ryosuke Kadono
Koichiro Shimomura
Kenji Kojima
Patrick Strasser
Naritoshi Kawamura
Akihiro Koda
Hiroshi Fujimori
Shunsuke Makimura
Yasuhisa Nemoto
Yasuo Kobayashi
Jumpei Nakamura
Kusuo Nishiyama
Toshiro Irie
Yutaka Taniguchi		Yutaka Ikedo
		
Masanori Miyazaki		Ichihiro Yamauchi
		Takashi Nagatomo		Yohei Nakatsugawa
		Yoshitomo Takahashi		Masatoshi Hiraishi
		Motonobu Tampo
		Koji Hamada		
Li Hua		
Masato Tabe
			
JAEA
		
Wataru Higemoto		Takashi Ito182

MLF Operations in 2013

*additional duties

CROSS-Tokai Staff 2013
Director

Yasuhiko Fujii

Science Cordinators		

Masatoshi Sato		

Yoshiaki Fukushima

		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		
		

Tetsuya Kuroda
Shinichi Machida
Masato Matsuura
Noboru Miyata
Tazuko Mizusawa
Toshiaki Morikawa
Taketo Moyoshi
Koji Munakata
Akiko Nakao
Kazuki Ohishi
Keiichi Ohuchi
Nobuo Okazaki
Masae Sahara
Yoshifumi Sakaguchi
Kaoru Sato
Sayaka Suzuki
Taiki Tominaga
Takeshi Yamada

		
		
		
		
		
		

Katsumi Kunigihara
Junko Ohta
Rei Ohuchi
Emi Takaha
Aya Yamada
Shinichi Yamaguchi

Neutron R&D Division
Head
Jun-ichi Suzuki
Head (Deputy) Kenichi Funakoshi		Jun Abe		
Kazuhiro Akutsu
		Tadashi Futagami
		Takayasu Hanashima		Hideyuki Hiramatsu		Kazuki Iida		
Kazuhiko Ikeuchi
		Motoyuki Ishikado
		Takayoshi Ito		
Hiroki Iwase		
Kazuya Kamazawa
		Satoshi Kasai		Yukihiko Kawamura		Hiroshi Kira		Koji Kiriyama
		Akifumi Kishi
		
Makoto Kobayashi

Health and Safety Division
Head

Toshiyuki Yamashita

Utilization Promotion Division
Head
Head (Deputy)
Adviser
		
		
		
		

Junichi Sato
Garry John Foran
Toru Matoba
Toshiki Asai
Yutaka Ebara
Asami Inoue
Megumi Kawakami

MLF Operations in 2013

183

Admin and Finance Division
Head
Head(Deputy)		184

MLF Operations in 2013

Yasuo Seishi
Masaru Yokoyama
Mika Gunji

		
		
		

Takahiro Koizumi
Mutsumi Shiraishi
Tomoyuki Yabana

Committees and Meetings
Materials and Life Science Facility Advisory Board
物質・生命科学実験施設利用委員会
Kazuya Aizawa
Japan Atomic Energy Agency, Japan
Jun Akimitsu
Aoyama Gakuin University, Japan
Masatoshi AraiJapan Atomic Energy Agency, Japan
Koichiro Asahi
Tokyo Institute of Technology, Japan
Yasuhiko Fujii
Comprehensive Research Organization for Science and Society, Japan
Masatoshi Futakawa
Japan Atomic Energy Agency, Japan
Makoto Hayashi
IBARAKI Prefectural Government, Japan
Shinichi Itoh
High Energy Accelerator Research Organization, Japan
Masahiko Iwasaki
RIKEN, Japan
Ryosuke KadonoHigh Energy Accelerator Research Organization, Japan
Takashi Kamiyama
High Energy Accelerator Research Organization, Japan
Toshiji Kanaya
Kyoto University, Japan
Mikio Kataoka
Nara Institute of Science and Technology, Japan
Takashi KatoJapan Atomic Energy Agency, Japan
Yukinobu Kawakita
Japan Atomic Energy Agency, Japan
Youji Koike
Tohoku University, Japan
Yasuhiro Miyake
High Energy Accelerator Research Organization, Japan
Toshiya Otomo
High Energy Accelerator Research Organization, Japan
Taku Sato
Tohoku University, Japan
Hideki Seto
High Energy Accelerator Research Organization, Japan
Mitsuhiro Shibayama (Chair) University of Tokyo, Japan
Masaaki Sugiyama
Kyoto University, JapanJun Sugiyama
Toyota Central R&D Labs., Inc., Japan
Wataru Utsumi
Japan Atomic Energy Agency, Japan
Toshio Yamaguchi
Fukuoka University, Japan
Term of board appointments: 1 April 2013 - 31 March 2015

Neutron Instrument Proposal Review Committee
中性子実験装置部会
Masatoshi Arai
Koichiro Asahi
Masatoshi Futakawa
Muneyuki Imafuku
Takashi Kamiyama
Hideaki Kitazawa
Yoshiaki Kiyanagi (Chair)
Yukio Morii
Yukio Morimoto
Kenji Nakajima
Kenji Ohoyama

Japan Atomic Energy Agency, JapanTokyo Institute of Technology, Japan
Japan Atomic Energy Agency, JapanTokyo City University, Japan
High Energy Accelerator Research Organization, Japan
National Institute for Material Science, Japan
Nagoya University, JapanThe Science and Technology Promotion Foundation of Ibaraki, Japan
Kyoto University, Japan
Japan Atomic Energy Agency, Japan
Tohoku University, JapanMLF Operations in 2013185

Toshiya Otomo
Mamoru Sato
Hideki Seto
Junichi Suzuki
Naoya Torikai
Hideki Yoshizawa

High Energy Accelerator Research Organization, Japan
Yokohama City University, Japan
High Energy Accelerator Research Organization, Japan
Comprehensive Research Organization for Science and Society, Japan
Mie University, Japan
University of Tokyo, Japan

Term of committee appointments: 1 April 2011 - 31 March 2013

Neutron Science Proposal Review Committee
中性子課題審査部会
Yoshiaki Akiniwa
Koichi Akita
Masatoshi Arai
Takahisa Arima
Samrath Chaplot
Sung-Min Choi
Sergey Danilkin
Yoshiaki Fukushima
Masatoshi Futakawa
Makoto Hayashi
Yasushi Idemoto
Michael James
Hiroyuki Kagi
Takashi Kamiyama
Yuji Kawabata
Yukinobu Kawakita
Brendan Kennedy
Guinyun Kim
Paul Langan
Seung-Hun Lee
Masaaki Matsuda
Yasuhiro Miyake
Yukio Morii
Yukio Noda
Toshiya Otomo
Anna Paradowska
Je-Geun Park
Mamoru Sato
Hideki Seto
Shinichi Shamoto
Hirohiko. M. Shimizu
Masaaki Sugiyama
Jun-ichi Suzuki
Toshio Yamaguchi (Chair)
Albert Young186

MLF Operations in 2013

Yokohama National University, Japan
Japan Atomic Energy Agency, Japan
Japan Atomic Energy Agency, Japan
University of Tokyo, Japan
Bhabha Atomic Research Centre, India
Korea Advanced Institute of Science and Technology, Korea
Australian Nuclear Science and Technology Organization, Australia
Comprehensive Research Organization for Science and Society, Japan
Japan Atomic Energy Agency, Japan
Ibaraki Prefectural Government, JapanTokyo University of Science, Japan
Australian Synchrotron, Australia
University of Tokyo, Japan
High Energy Accelerator Research Organization, Japan
Kyoto University, Japan
Japan Atomic Energy Agency, Japan
University of Sydney, Australia
Kyungpook University, Korea
Oak Ridge National Laboratory, USA
University of Virginia, USA
Oak Ridge National Laboratory, USA
High Energy Accelerator Research Organization, JapanThe Science and Technology Promotion Foundation of Ibaraki, Japan
Tohoku University, Japan
High Energy Accelerator Research Organization, Japan
Australian Nuclear Science and Technology Organization, Australia
Seoul National University, Korea
Yokohama City University, Japan
High Energy Accelerator Research Organization, Japan
Japan Atomic Energy Agency, Japan
Nagoya University, Japan
Kyoto University, Japan
Comprehensive Research Organization for Science and Society, Japan
Fukuoka University, Japan
North Carolina State University, USATerm of committee appointments: 1 April 2013 - 31 March 2015

JAEA Research Proposal Advisory Committee
J-PARC物質・生命科学実験施設におけるJAEA研究課題諮問委員会
Masatoshi AraiJapan Atomic Energy Agency, Japan
Toshiharu Fukunaga
Kyoto University, Japan
Mitsuhiro Hirai
Gunma University, Japan
Takashi Kato (Chair)Japan Atomic Energy Agency, Japan
Yuji Kawabata
Kyoto University, Japan
Yukinobu Kawakita
Japan Atomic Energy Agency, Japan
Hideaki Kitazawa
National Institute for Material Science, Japan
Yoshiaki Kiyanagi
Nagoya University, Japan
Michiyasu Mori
Japan Atomic Energy Agency, Japan
Yoichi MurakamiHigh Energy Accelerator Research Organization, Japan
Kenji Nakajima
Japan Atomic Energy Agency, Japan
Hiroyuki Oigawa
Japan Atomic Energy Agency, Japan
Taku Sato
University of Tokyo, Japan
Hideki Seto
High Energy Accelerator Research Organization, Japan
Shinichi Shamoto
Japan Atomic Energy Agency, Japan
Hirohiko M. Shimizu
Nagoya University, Japan
Junichi Suzuki
Comprehensive Research Organization for Science and Society, Japan
Keisuke Tanaka
Meijo University, Japan
Yo Tomota
Ibaraki University, Japan
Eiko Torikai
University of Yamanashi, Japan
Kazuyoshi YamadaHigh Energy Accelerator Research Organization, Japan
Term of committee appointments: 1 April 2011 - 31 March 2014

Neutron Program Advisory Committee
中性子共同利用実験審査委員会
Koichiro Asahi
Masaki Azuma
Michihiro Furusaka
Yasushi Idemoto
Shinichi Itoh
Kazuaki Iwasa
Ryosuke Kadono
Hiroshi Kageyama
Takashi Kamiyama
Toshiji Kanaya
Mikio Kataoka
Yukinobu Kawakita
Reiji Kumai
Yutaka Moritomo

Tokyo Institute of Technology, JapanTokyo Institute of Technology, Japan
Hokkaido University, JapanTokyo University of Science, Japan
High Energy Accelerator Research Organization, Japan
Tohoku University, Japan
High Energy Accelerator Research Organization, Japan
Kyoto University, Japan
High Energy Accelerator Research Organization, Japan
Kyoto University, Japan
Nara Institute of Science and Technology, Japan
Japan Atomic Energy Agency, Japan
High Energy Accelerator Research Organization, Japan
University of Tsukuba, JapanMLF Operations in 2013187

Youichi Murakami
Toshiya Otomo (Chair)
Hideki Seto
Mitsuhiro Shibayama
Hirohiko M. Shimizu
Masaaki Sugiyama
Noboru Yamamoto

High Energy Accelerator Research Organization, Japan
High Energy Accelerator Research Organization, Japan
High Energy Accelerator Research Organization, Japan
University of Tokyo, Japan
High Energy Accelerator Research Organization, Japan
Kyoto University, Japan
High Energy Accelerator Research Organization, Japan

Term of committee appointments: 1 April 2013 - 31 March 2015

Muon Instrument Proposal Review Committee
ミュオン実験装置部会
Masatoshi Arai
Koichiro Asahi (Chair)
Masatoshi Futakawa
Wataru Higemoto
Masahiko Iwasaki
Ryosuke Kadono
Takashi Kato
Kenji Kojima
Kenya Kubo (Chair)
Yoshitaka Kuno
Yasuhiro Miyake
Nobuhiko Nishida
Hiroyuki Nojiri
Toru Ogitsu
Koichiro Shimomura
Yasunori Yamazaki

Japan Atomic Energy Agency, JapanTokyo Institute of Technology, Japan
Japan Atomic Energy Agency, Japan
Japan Atomic Energy Agency, JapanRIKEN, Japan
High Energy Accelerator Research Organization, Japan
Japan Atomic Energy Agency, Japan
High Energy Accelerator Research Organization, Japan
International Christian University, Japan
Osaka University, Japan
High Energy Accelerator Research Organization, JapanTokyo Institute of Technology, Japan
Tohoku University, Japan
High Energy Accelerator Research Organization, Japan
High Energy Accelerator Research Organization, JapanRIKEN, Japan

Term of committee appointments: 1 April 2013 - 31 March 2015

Muon Science Proposal Review Committee
ミュオン課題審査部会
Hiroshi Amitsuka
Masaharu Aoki
Masatoshi Arai
Koichiro Asahi
Alan Drew
Wataru Higemoto
Ryosuke Kadono
Takashi Kamiyama
Toshiji Kanaya
Yoh Kohori
Yoji Koike (Chair)
Kenji Kojima

188

MLF Operations in 2013

Hokkaido University, Japan
Osaka University, Japan
Japan Atomic Energy Agency, JapanTokyo Institute of Technology, Japan
University of London, UK
Japan Atomic Energy Agency, Japan
High Energy Accelerator Research Organization, Japan
High Energy Accelerator Research Organization, Japan
Kyoto University, Japan
Chiba University, Japan
Tohoku University, Japan
High Energy Accelerator Research Organization, Japan

Tadashi Koseki
Kenya Kubo
Reiji Kumai
Roderick Macrae
Yasuyuki Matsuda
Yasuhiro Miyake
Seiji Miyasita
Yasuo Nozue
Toshiya Otomo
Hideki Seto
Koichiro Shimomura
Yoko Sugawara
Shinji Tsuneyuki
Kazuyoshi YoshimuraHigh Energy Accelerator Research Organization, Japan
International Christian University, Japan
High Energy Accelerator Research Organization, Japan
Marian University, USA
University of Tokyo, Japan
High Energy Accelerator Research Organization, Japan
University of Tokyo, Japan
Osaka University, Japan
High Energy Accelerator Research Organization, Japan
High Energy Accelerator Research Organization, Japan
High Energy Accelerator Research Organization, Japan
Kitazato University, Japan
University of Tokyo, Japan
Kyoto University, Japan

Term of committee appointments: 1 April 2013 - 31 March 2015

Muon Program Advisory Committee
ミュオン共同利用実験審査委員会
Hiroshi Amitsuka
Hokkaido University, Japan
Masaharu Aoki
Osaka University, Japan
Masatoshi AraiJapan Atomic Energy Agency, Japan
Koichiro Asahi
Tokyo Institute of Technology, Japan
Wataru Higemoto
Japan Atomic Energy Agency, Japan
Ryosuke Kadono (Chair)High Energy Accelerator Research Organization, Japan
Toshiji Kanaya
Kyoto University, Japan
Yoh Kobori
Chiba University, Japan
Yoji Koike
Tohoku University, Japan
Kenji Kojima
High Energy Accelerator Research Organization, Japan
Tadashi Koseki
High Energy Accelerator Research Organization, Japan
Kenya Kubo
International Christian University, Japan
Reiji Kumai
High Energy Accelerator Research Organization, Japan
Yasuyuki Matsuda
University of Tokyo, Japan
Yasuhiro Miyake
High Energy Accelerator Research Organization, Japan
Seiji Miyashita
University of Tokyo, Japan
Yasuo Nozue
Osaka University, Japan
Toshiya Otomo
High Energy Accelerator Research Organization, Japan
Hideki Seto
High Energy Accelerator Research Organization, Japan
Koichiro Shimomura
High Energy Accelerator Research Organization, Japan
Yoko Sugawara
Kitazato University, Japan
Shinji Tsuneyuki
University of Tokyo, Japan
Kazuyoshi Yoshimura
Kyoto University, Japan
Term of committee appointments: 1 April 2013 - 31 March 2015

MLF Operations in 2013189

Selection Committee (CROSS)
選定委員会
Toshio Akai
Jun Akimitsu
Koichiro Asahi
Hidetoshi Fukuyama (Chair)
Makoto Hayashi
Shinichi Kamei
Toshiji Kanaya
Mikio Kataoka
Naoki Kishimoto
Tomoko Nakanishi(*)
Kazumi Nishijima
Taku Sato
Mitsuhiro Shibayama
Masaaki Sugiyama
Masaki Takada
Kiyoyuki Terakura
Toshio Yamaguchi

Mitubishi Rayon co.,Ltd., Japan
Aoyama Gakuin University, JapanTokyo Institute of Technology, JapanTokyo University of Science, Japan
IBARAKI Prefectural Government, Japan
Mitsubishi Research Institute Inc., Japan
Kyoto University, Japan
Nara Institute of Science and Technology, Japan
National Institute of Material Science, Japan
University of Tokyo, Japan
Mochida Pharmaceutical co.,Ltd., Japan
Tohoku University, Japan
University of Tokyo, Japan
Kyoto University, JapanRIKEN, Japan
National Institute of Advanced Industrial Science and Technology, Japan
Fukuoka University, Japan* Until 28 February 2014
Term of committee appointments: 1 May 2013 - 31 March 2015190

MLF Operations in 2013

Neutron Advisory Committee (NAC)

NAC-2014 convened 10-11 Feb 2014 at the KEK Tokai campus building, Tokai
List of NAC-2014 Members
Kurt N. Clausen (Chair)Phillip Ferguson
Mahn Won Kim
Yoshiaki Kiyanagi
Dan A. Neumann
Robert Robinson
Uschi Steigenberger
Werner Wagner

Paul Scherrer Institute, Switzerland
Oak Ridge National Laboratory, USA
Korea Advanced Institute of Science and Technology, Korea
Nagoya University, Japan
National Institute of Standards and Technology, USA
Australian Nuclear Science and Technology Organization, Australia
Science and Technology Facilities Council, UK
Paul Scherrer Institute, Switzerland

Group photo of NAC-2014

MLF Operations in 2013191

Muon Science Advisory Committee (MuSAC)

MuSAC-12 convened 27-28 Feb 2014 at the KEK Tokai Campus building, Tokai
List of MuSAC-12 Members
Hiroshi Amitsuka
Toshiyuki Azuma
Klaus P. Jungman
Elvezio Morenzoni (Chair)
Yasuo Nozue
Francis Pratt
Jeff E. Sonier
Jun Sugiyama

192

MLF Operations in 2013

Hokkaido University, JapanRIKEN, Japan
University of Groningen, Netherlands
Paul Scherrer Institute, Switzerland
Osaka University, Japan
ISIS, UK
Simon Fraser University, Canada
Toyota Central R&D Labs., Inc., Japan

Workshops in 2013
With the increasing level of scientific activity at the facility, the number and scope of researchworkshops held under the auspices of the MLF rapidly expanded in 2013.

Conferences and workshops held jointly by J-PARC MLF and CROSS-Tokai
2nd IMSS Science Festa, 5th MLF Symposium, 31th PF Symposium
18–19 Mar. 2014, Tsukuba International Congress Center, Tsukuba

Workshops co-sponsored by J-PARC Center, CROSS-Tokai and other organizations
JSNS Annual Meeting 2013
12–13 Dec. 2013, Sawayaka Chiba Kenmin Plaza, Chiba

13th Japan-Korea Meeting on Neutron Science
16–18 Feb. 2014, Lotte Buyeo Resort, Korea

MLF Operations in 2013193

元素戦略プロジェクト＜研究拠点形成型＞・大型研究施設（CMSI・SPring-8・J-PARC・KEK）連携
シンポジウム2014 ～大型研究施設を利用した物質・材料研究の課題共有と共創～
28 Feb. – 1 Mar. 2014, The University of Tokyo Kasiwa Campus, Chiba

Neutrons in Biology
27 Mar. 2014, Nuclear Science Research Institute, JAEA, Tokai

Workshops co-sponsored by J-PARC
2nd ANNRI Workshop
23 Aug. 2013, Ibaraki Quantum Beam Center, Tokai

Workshops held by KEK
4th Progress report meeting of J-PARC MUSE
6 Jun. 2013, KEK Tokai campus, Tokai (50 participants, 21 presentations)

CMRC workshop (Iron Pnictide-Oxides)
8 Jul. 2013, KEK Tsukuba campus, Tsukuba(50 participants, 8 presentations)Light and Particle Beams in Materials Science (LPBMS2013)
29–31 Aug. 2013, Tsukuba International Congress Center, Tsukuba(200 participants, 62 oral and 126 poster presentations)

7th collaboration meeting on muon g-2/EDM experiment at J-PARC
5–7 Dec. 2013, KEK Tsukuba campus and Tokai campus, Ibaraki(50 participants, 36 presentations)194

MLF Operations in 2013

Workshop co-sponsored and supported by CROSS-Tokai
2013 Workshop on Materials Science
31 Jul. 2013, KENKYUSHA EIGO Center, Tokyo

2013 Ibaraki Society for Promotion of Use of Neutrons Workshop
on Texture Evaluation of Metal Material
28 Aug. 2013, KENKYUSHA EIGO Center, Tokyo

1st 2013 Workshop on Neutron Scattering from Soft Matter
6 Sep. 2013, KENKYUSHA EIGO Center, Tokyo

1st 2013 Workshop on Residual Stress and Strain
17 Sep. 2013, KENKYUSHA EIGO Center, Tokyo

2013 Workshop on Metallographic Structure
4 Oct. 2013, KENKYUSHA EIGO Center, Tokyo

1st 2013 Workshop on Structural Biology
9 Oct. 2013, ESSAM Kanda Hole, Tokyo

2013 Ibaraki Society for Promotion of Use of Neutrons Workshop
on Texture Evaluation of Metal Material
15 Oct. 2013, Ibaraki Quantum Beam Center, Tokai

2012 The CROSS Trial Use and Ibaraki Beam Line Users Meeting
18 Oct. 2013, Kagaku-kaikan Hall, Tokyo

MLF Operations in 2013195

2013 Ibaraki Society for Promotion of Use of Neutrons Meetingon in situ of Magnet materials structure analysis
22 Oct. 2013, KENKYUSHA EIGO Center, Tokyo

2013 Workshop on Non-destructive Visualization and Analysis Methods
5 Nov. 2013, KENKYUSHA EIGO Center, Tokyo

2013 Ibaraki Society for Promotion of Use of Neutrons Meeting on in situ of Battery materials
2 Dec. 2013, KENKYUSHA EIGO Center, Tokyo

2013 Workshop on Magnetic Materials
20 Dec. 2013, KENKYUSHA EIGO Center, Tokyo

2013 Workshop on Surfaces and Interfaces
17 Jan. 2014, ESSAM Kanda Hall, Tokyo

2013 Ibaraki Society for Promotion of Use of Neutrons Workshop
on Organic and Polymeric Materials Neutron Structure Elucidation
30 Jan. 2014, KENKYUSHA EIGO Center, Tokyo

5th Workshop on Analytical Methods In Small Angle Scattering
3 Mar. 2014, KENKYUSHA EIGO Center, Tokyo196

MLF Operations in 2013

2nd 2013 Workshop on Soft Matter Neutron Scattering
4 Mar. 2014, ESSAM Kanda Hall, Tokyo

2nd 2013 Workshop on Residual Stress and Strain
7 Mar. 2014, KENKYUSHA EIGO Center, Tokyo

3rd 2013 Workshop on Soft Matter Neutron Scattering
14 Mar. 2014, ESSAM Kanda Hole, Tokyo

2nd 2013 Workshop on Structural Biology
17 Mar. 2014, KENKYUSHA EIGO Center, Tokyo

MLF Operations in 2013

197

Workshops held by CROSS-Tokai
The 7th CROSSroads of Users and J-PARC Functional Interfaces and Reactive Surfaces
20–21 Aug. 2013, Ibaraki Quantum Beam Center, Tokai

The 8th CROSSroads of Users and J-PARC
Neutron Scattering and Nano-second Dynamics - What is the future?
11–12 Nov. 2013, Ibaraki Quantum Beam Center, Tokai

The 9th CROSSroads of Users and J-PARC Superconductivity, Magnetism and Frustration
3–5 Dec. 2013, KEK Tokai campus, Tokai

The 10th CROSSroads of Users and J-PARC Frontier Research on Bio-membranes and Colloids
18–19 Dec. 2013, Ibaraki Quantum Beam Center, Tokai198

MLF Operations in 2013

Seminars and Courses in 2013
Seminars co-convened and supported by CROSS-Tokai with other organizations
Industrial Applications of Neutron Scattering
27 Sep. 2013, Furukawa Electric Co. Ltd., Kanagawa
Synchrotron Radiation-Neutron Linkage Use Seminar in Aichi
15 Jan. 2014, Aichi Center for Industry and Science Technology, Aichi
Industrial Applications of Neutron Scattering
21 Jan. 2014, Nitto Denko Corporation, Osaka
Seminar About The Industrial Application by The Complementarity Use of Synchrotron Radiation
and The Neutron in Kobe
24 Feb. 2014, Hyogo Prefecture Citizens’ Hall, Hyogo

Short Courses co-sponsored by J-PARC Center, CROSS-Tokai and other organizations
Z-Code Training Course
25–26 Mar. 2014, LMJ Tokyo, Tokyo

MLF Operations in 2013199

Schools in 2013
KEK Summer Challenge
16–25 Aug. 2013, KEK, Tsukuba

Credit : KEK

200

MLF Operations in 2013

Award List
The JSNS Outstanding Achievement Prize
Neutron Optics and the Instrumentations
The Japanese Society for Neutron Science
Toru Ebisawa, December 2013
The JSNS Young Researcher Prize
Development of the Magnetic Field Imaging using
Polarized Pulsed Neutrons
The Japanese Society for Neutron Science
Takenao Shinohara, December 2013
The JSNS Young Researcher Prize
Development of Model-free Analysis Method on
Quasi-elastic Neutron Scattering and Application to
Liquid Water
The Japanese Society for Neutron Science
Tatsuya Kikuchi, December 2013
The JSNS Technology Prize
Development of a Chopper Spectrometer with a
Pulse-shaping Chopper at a Pulsed Source
The Japanese Society for Neutron Science
Kenji Nakajima, Seiko Kawamura, Katsuhiko
Yoshida, Mitsutaka Nakamura, Ryoichi Kajimoto,and Masatoshi Arai, December 2013平成 24 年度 日本中間子科学会若手奨励賞µSR による鉄系超伝導体 CaFe 1-xCox AsF における超伝導と
磁性の研究
竹下聡史
平成 25 年 3 月 26 日
平成 26 年度 科学技術分野の文部科学大臣表彰
若手科学者賞(The Commendation for Science and Technology by
the Minister of Education, Culture, Sports, Scienceand Technology: The Young Scientists’ Prize)
地球深部における鉱物中の水素結合と同位体効果の研究
佐野亜沙美
平成 26 年 4 月 15 日
平成 25 年度理事長表彰 研究開発功績賞（日本原子力研究開発機構）
244
246
大強度中性子ビームを用いた Cm 及び Cm の中性子捕獲断面積の高精度化研究
木村敦、古髙和禎、原かおる 、原田秀郎、
北谷文人、小泉光生、中村詔司、藤暢輔
平成 25 年 10 月 15 日
平成 25 年度理事長表彰 創意工夫功労賞（日本原子力研究開発機構）
10
大強度パルス中性子対応 ZnS/ B 2O 3 セラミックシンチレータ検出器の開発とその実用化
中村龍也、藤健太郎、坂佐井馨、曽山和彦、
美留町厚、海老根守澄
平成 25 年 10 月 15 日
平成 25 年度理事長表彰 理事長奨励賞（日本原子力研究開発機構）
国家課題対応型研究開発推進事業―光・量子融合連携研究
開発プログラム―［実用製品中の熱、構造、磁気、元素の直接観察による革新エネルギー機器の実現］
新井正敏
平成 25 年 10 月 15 日

MLF Operations in 2013201

MLF Publication 2013
1

K. Aizawa, W. Gong, S. Harjo, J. Abe, T. Iwahashi, and T.
Kamiyama
In-Situ Neutron Diffraction Study on Tensile Behavior of LPSO
Mg-Zn-Y Alloys
Materials Transactions 54 1083 (2013)10

M. Fujita, C. D. Frost, S. M. Bennington, R. Kajimoto, M.
Nakamura, Y. Inamura, F. Mizuno, K. Ikeuchi, and M. Arai
Temperature Dependence of Spin Excitations in the Frustrated
Spin Chain System CuGeO3
Journal of the Physical Society of Japan 82 84708 (2013)

2

H. Anzai, A. Ino, M. Arita, H. Namatame, M. Taniguchi, M.
Ishikado, K. Fujita, S. Ishida, and S. Uchida
Relation between the nodal and antinodal gap and criticaltemperature in superconducting Bi2212
Nature Communications 4 1815 (2013)11

S. Fujiwara, T. Yamada, T. Matsuo, N. Takahashi, K. Kamazawa, Y.
Kawakita, and K. Shibata
Internal Dynamics of a Protein That Forms the Amyloid Fibrils
Observed by Neutron Scattering
Journal of the Physical Society of Japan 82 SA019 (2013)3

M. Arai, R. Kajimoto, M. Nakamura, Y. Inamura, K. Nakajima, K.
Shibata, N. Takahashi, J. Suzuki, S. Takata, T. Yamada, and S. Itoh
Recent Developments of Instruments in a Spallation Neutron
Source at J-PARC and Those Prospects in the Future
Journal of the Physical Society of Japan 82 SA024 (2013)

12

S. Ghosh, E. Ohtani, K. D. Litasov, A. Suzuki, D. Dobson, and K.
Funakoshi
Effect of water in depleted mantle on post-spinel transition andimplication for 660 km seismic discontinuity
Earth and Planetary Science Letters 371–372 103 (2013)4

H. Arai, K. Mori, Y. Onodera, T. Fukunaga, M. Yonemura, T.
Kamiyama, M. Nagao, and I. S. Torii
Expectation of Analysis Using BL09/SPICA, the World’s First
Neutron Beamline Dedicated for Battery Analysis
世界初の蓄電池専用中性子ビームライン BL09/SPICA を用いた解析への期待（超の世界）
Journal of Society of Automotive Engineers of Japan/ 自動車技術
67 108 (2013)

13

W. Gong, K. Aizawa, S. Harjo, J. Abe, T. Iwahashi, and T.
Kamiyama
Neutron Diffraction on LPSO Structure in Mg-Zn-Y Alloys
Materials Transactions 54 974 (2013)

14

W. Gong, Y. Tomota, Y. Adachi, A. M. Paradowska, J. F. Kelleher,
and S. Y. Zhang
Effects of ausforming temperature on bainite transformation,
microstructure and variant selection in nanobainite steel
Acta Materialia 61 4142 (2013)15

T. Hagiwara, H. Yamamura, K. Nomura, and M. Igawa
Relationship between crystal structure and oxide-ionconductionin Ln2Zr2O7 (Ln=Eu, Nd and La) system deduced by neutron and
X-ray diffraction
Journal of the Ceramic Society of Japan 121 205 (2013)16

T. Hanna, S. Matsuishi, K. Kodama, T. Otomo, S. Shamoto, and H.
HosonoFrom antiferromagnetic insulator to ferromagnetic metal: Effectsof hydrogen substitution in LaMnAsO
Physical Review B 87 20401 (2013)

17

K. Y. Hara, H. Harada, Y. Toh, and J. Hori
γ-Flash suppression using a gated photomultiplier assembled withan LaBr3(Ce) detector to measure fast neutron capture reactions
Nuclear Instruments and Methods in Physics Research Section A
723 121 (2013)18

M. Harada, J. D. Parker, T. Sawano, H. Kubo, T. Tanimori, T.
Shinohara, F. Maekawa, and K. Sakai
Quantitative Measurement of Element Distributions using the
Neutron-transmission Resonance-absorption Method
Physics Procedia 43 314 (2013)19

S. Harjo, N. Tsuchida, W. Gong, J. Abe, and K. Aizawa
TRIP Steel Deformation Behavior by Neutron Diffraction
Materials Research Society Symposium Proceedings 1528 (2013)20

S. Hasegawa, S. Takahashi, H. Iwase, S. Koizumi, M. Ohnuma,
and Y. Maekawa
Crystal morphology-dependent graft polymerization in poly(ether
ether ketone) films
Polymer 54 2895 (2013)21

H. Hayashida, M. Takeda, D. Yamazaki, R. Maruyama, K. Soyama,

5

6

H. Arita, K. Mitamura, M. Kobayashi, N. L. Yamada, H. Jinnai,
and A. Takahara
Chain-mixing behavior at interface between polystyrene brushes
and polystyrene matrices
Polymer Journal 45 117 (2013)

7

S. Asai, R. Okazaki, I. Terasaki, Y. Yasui, W. Kobayashi, A. Nakao,
K. Kobayashi, R. Kumai, H. Nakao, Y. Murakami, N. Igawa,
A. Hoshikawa, T. Ishigaki, O. Parkkima, M. Karppinen, and H.
YamauchiSpin State of Co3+ in LaCo 1-xRh xO 3 Investigated by Structural
Phenomena
Journal of the Physical Society of Japan 82 114606 (2013)

8

P. Bakule, G. A. Beer, D. Contreras, M. Esashi, Y. Fujiwara, Y.
Fukao, S. Hirota, H. Iinuma, K. Ishida, M. Iwasaki, T. Kakurai,
S. Kanda, H. Kawai, N. Kawamura, G. M. Marshall, H. Masuda,
Y. Matsuda, T. Mibe, Y. Miyake, S. Okada, K. Olchanski, A. Olin,
H. Onishi, N. Saito, K. Shimomura, P. Strasser, M. Tabata, D.
Tomono, K. Ueno, K. Yokoyama, and S. Yoshida
Measurement of muonium emission from silica aerogel
Progress of Theoretical and Experimental Physics 103C01 (2013)

9202

T. Arimori, N. Kawamoto, S. Shinya, N. Okazaki, M. Nakazawa, K.
Miyatake, T. Fukamizo, M. Ueda, and T. Tamada
Crystal structures of the catalytic domain of a novel glycohydrolase
family 23 chitinase from Ralstonia sp. A-471 reveals a uniquearrangement of the catalytic residues for inverting chitin hydrolysis
The Journal of Biological Chemistry 288 18696 (2013)

W. Chuajiw, M. Nakano, K. Takatori, T. Kojima, Y. Wakimoto, andY. Fukushima
Effects of amine, amine salt and amide on the behaviour ofcarbon dioxide absorption into calcium hydroxide suspension toprecipitate calcium carbonate
Journal of Environmental Sciences 25 2507 (2013)

MLF Operations in 2013

M. Kubota, T. Mizusawa, N. Yoshida, and Y. Sakaguchi
Design and Demonstration of a Neutron Spin Flipper for a New
Neutron Reflectometer SHARAKU at J-PARC
Physics Procedia 42 130 (2013)
22

T. Hemmi, S. Harjo, Y. Nunoya, H. Kajitani, N. Koizumi, K.
Aizawa, S. Machiya, and K. Osamura
Neutron diffraction measurement of internal strain in the firstJapanese ITER CS conductor sample
Superconductor Science and Technology 26 84002 (2013)23

M. Hiroi, T. Hisamatsu, T. Suzuki, K. Ohishi, Y. Ishii, and I.
WatanabeMuon spin relaxation study of spin-glass freezing in the Heusler
compound Ru1.9Fe0.1CrSi
Physical Review B 88 24409 (2013)24

K. Hirose, K. Furutaka, K. Y. Hara, H. Harada, A. Kimura, T. Kin,
F. Kitatani, M. Koizumi, S. Nakamura, M. Oshima, Y. Toh, M.
Igashira, T. Katabuchi, M. Mizumoto, T. Kamiyama, K. Kino, Y.
Kiyanagi, and J. Hori
Cross-section measurement of 237Np (n, γ) from 10 meV to 1 keV at
Japan Proton Accelerator Research Complex
Journal of Nuclear Science and Technology 50 188 (2013)

25

26

A. Hoshikawa, T. Ishigaki, and M. Yonemura
Development of Automatic Sample Exchange and Transfer System
in iMATERTAiMATERIA における自動試料交換搬送機構の開発
Hamon/ 波紋 23 204 (2013)
N. Hoshino, F. Iijima, G. N. Newton, N. Yoshida, T. Shiga, H.
Nojiri, A. Nakao, R. Kumai, Y. Murakami, and H. Oshio
Three-way Switching in a Cyanide-bridged [FeCo] Chain
熱・光によって磁性・電気伝導性が変化するシアン化物イ
オン架橋混合原子価 [Fe-Co] 一次元鎖錯体
Photon Factory News 31 12 (2013)

27

S. Iimura, S. Matsuishi, M. Miyakawa, T. Taniguchi, K. Suzuki,
H. Usui, K. Kuroki, R. Kajimoto, M. Nakamura, Y. Inamura, K.
Ikeuchi, S. Ji, and H. Hosono
Switching of intra-orbital spin excitations in electron-doped ironpnictide superconductors
Physical Review B 88 60501 (2013)28

Y. Ikedo, Y. Miyake, K. Shimomura, P. Strasser, N. Kawamura,
K. Nishiyama, S. Makimura, H. Fujimori, A. Koda, J. Nakamura,
T. Nagatomo, Y. Kobayashi, T. Adachi, A. D. Pant, T. Ogitsu,
T. Nakamoto, K. Sasaki, H. Ohata, R. Okada, A. Yamamoto, Y.
Makida, M. Yoshida, T. Okamura, R. Okubo, W. Higemoto, T. U.
Ito, K. Nakahara, and K. Ishida
Positron separators in Superomega muon beamline at J-PARC
Nuclear Instruments and Methods in Physics Research Section B
317 365 (2013)

29

K. Ikeuchi, R. Kajimoto, F. Mizuno, M. Fujita, Y. Inamura, M.
Nakamura, K. Nakajima, K. Aizawa, and M. Arai
Anisotropic spin excitations in spin-Peierls CuGeO3
Journal of the Korean Physical Society 63 333 (2013)

30

K. Ikeuchi, M. Nakamura, R. Kajimoto, and M. Arai
Optimization of a Fermi Chopper for an Inelastic Neutron
Spectrometer with Focusing Guide
Journal of the Physical Society of Japan 82 SA038 (2013)31

Y. Inamura, T. Nakatani, J. Suzuki, and T. Otomo
Development Status of Software “Utsusemi” for Chopper
Spectrometers at MLF, J-PARC
Journal of the Physical Society of Japan 82 SA031 (2013)32

M. Inutsuka, N. L. Yamada, K. Ito, and H. Yokoyama
High Density Polymer Brush Spontaneously Formed by the
Segregation of Amphiphilic Diblock Copolymers to the Polymer/
Water Interface
ACS Macro Letters 2 265 (2013)

33

T. U. Ito, W. Higemoto, T. D. Matsuda, A. Koda, and K.
Shimomura
Shallow donor level associated with hydrogen impurities in
undoped BaTiO3Applied Physics Letters 103 (2013)

34

S. ItohAnomalous Spin Diffusion in Two-Dimensional Percolating
Antiferromagnet
Journal of the Physical Society of Japan 82 SA022 (2013)

35

S. ItohAnomalous spin diffusion on the two-dimensional percolating
network in Rb2Mn0.6Mg0.4F4
Journal of the Korean Physical Society 63 310 (2013)

36

S. Itoh, Y. Endoh, T. Yokoo, D. Kawana, Y. Kaneko, Y. Tokura, andM. Fujita
Neutron Brillouin Scattering with Pulsed Spallation Neutron
Source – Spin-Wave Excitations from Ferromagnetic Powder
Samples –Journal of the Physical Society of Japan 82 43001 (2013)

37

S. Itoh, T. Yokoo, D. Kawana, and Y. Endoh
Neutron Brillouin Scattering on High Resolution Chopper
Spectrometer, HRC
Journal of the Physical Society of Japan 82 SA034 (2013)

38

S. Itoh, T. Yokoo, D. Kawana, H. Yoshizawa, T. Masuda, M. Soda,
T. J. Sato, S. Satoh, M. Sakaguchi, and S. Muto
Progress in High Resolution Chopper Spectrometer, HRC
Journal of the Physical Society of Japan 82 SA033 (2013)

39

K. Iwasa, H. Kobayashi, T. Onimaru, K. T. Matsumoto, N.
Nagasawa, T. Takabatake, S. Ohira-Kawamura, T. Kikuchi, Y.
Inamura, and K. Nakajima
Well-Defined Crystal Field Splitting Schemes and Non-Kramers
Doublet Ground States of f Electrons in PrT2Zn20 (T= Ir, Rh, andRu)
Journal of the Physical Society of Japan 82 43707 (2013)

40

X. Jin, T. Nakamoto, S. Harjo, T. Hemmi, T. Umeno, T. Ogitsu,
A. Yamamoto, M. Sugano, K. Aizawa, J. Abe, W. Gong, and T.
Iwahashi
Development of a cryogenic load frame for the neutron diffractometerat Takumi in Japan Proton Accelerator Research Complex
Review of Scientiﬁc Instruments 84 063106 (2013)

41

R. Kajimoto, K. Nakajima, S. Ohira-Kawamura, Y. Inamura, K.
Kakurai, T. Hokazono, S. Oozono, and T. Okuda
Effects of Mg, Ag, and Al Substitutions on Magnetic Excitations in
the Triangular-Lattice Antiferromagnet CuCrO2
Journal of the Physical Society of Japan 82 54702 (2013)

42

R. Kajimoto, M. Nakamura, Y. Inamura, K. Ikeuchi, S. Ji, K.
Nakajima, S. Ohira-Kawamura, W. Kambara, M. Sawabe, A.
Kamiya, K. Inoue, T. Futagami, M. Kobayashi, A. Kishi, K. Satou,
K. Aizawa, and M. Arai
Recent Improvement of the Signal-to-Noise Ratio on the Fermi
Chopper Spectrometer 4SEASONS
Journal of the Physical Society of Japan 82 SA032 (2013)

43

R. Kajimoto, M. Nakamura, K. Nakajima, and M. FujitaContamination from the next higher incident energy in inelastic

MLF Operations in 2013203

neutron scattering measurements with multiple incident energies
on chopper spectrometers
Nuclear Instruments and Methods in Physics Research Section A
729 365 (2013)
44

45

T. Kamiyama, M. Yonemura, S. Torii, M. Nagao, and Y. Ishikawa
J-PARC MLF BL08: 粉末中性子回折装置
Photon Factory News 30 35 (2013)46

N. Kawamura, A. Toyoda, M. Aoki, N. Saito, S. Mihara, K.
Shimomura, and Y. Miyake
The H line: a brand new beam line for fundamental physics at the
J-PARC muon facility
Journal of Physics: Conference Series 408 12072 (2013)

47

K. Sasaki, M. Sugano, H. Iinuma, T. Ogitsu, N. Saito, K.
Shimomura, and A. Yamamoto
Development status of superconducting solenoid for the MuHFS
experiment at the J-PARC
Journal of Physics: Conference Series 408 12074 (2013)

48

T. Kikuchi, K. Nakajima, S. Ohira-Kawamura, Y. Inamura, O.
Yamamuro, M. Kofu, Y. Kawakita, K. Suzuya, M. Nakamura, and
M. AraiMode-distribution analysis of quasielastic neutron scattering andapplication to liquid waterPhysical Review E 87 62314 (2013)

49

H. Kinoshita, M. Kaminaga, K. Haga, A. Terada, and R. Hino
Experimental study on heat transfer and pressure drop in mercury
flow system for spallation neutron source
Journal of Nuclear Science and Technology 50 400 (2013)

50

Y. Kobayashi, T. Iida, K. Suzuki, T. Kawamata, M. Itoh, and M.
Sato75
As NQR and NMR Studies on the Superconducting State of
Ca10Pt4As8(Fe1−xPtxAs)10
Journal of the Physical Society of Japan 83 014712 (2013)

51

Y. Kobayashi, A. Ichikawa, M. Toyoda, M. Itoh, and M. Sato
In-plane anisotropy of the magnetic and the electric properties of
the Fe pnictide Ba(Fe1−xCox)2As2
Journal of the Korean Physical Society 63 481 (2013)

52

Y. Kobayashi, S. Saiki, S. Kototani, M. Itoh, and M. Sato
Phase separation of antiferromagnetism and superconductivity in
RbxFe2−ySe2 observed by using Rb NMR
Journal of the Korean Physical Society 63 448 (2013)

53

K. Kodama, N. Igawa, S. Shamoto, K. Ikeda, H. Oshita, N.
Kaneko, T. Otomo, and K. Suzuya
Local Lattice Distortion Caused by Short Range Charge Orderingin LiMn2O4
Journal of the Physical Society of Japan 82 94601 (2013)

54

M. Kofu, T. Kajiwara, J. S. Gardner, G. G. Simeoni, M. Tyagi, A.
Faraone, K. Nakajima, S. Ohira-Kawamura, M. Nakano, and O.
Yamamuro
Magnetic relaxations in a Tb-based single molecule magnet
studied by quasielastic neutron scattering
Chemical Physics 427 147 (2013)

55

204

T. Kamiyama, M. Yonemura, S. Torii, M. Nagao, and Y. Ishikawa
Application of Pulsed Neutron for Battery Research
パルス中性子で何ができるか : 蓄電池
Ionizing radiation/ 放射線 39 65 (2013)

M. Kofu, O. Yamamuro, T. Kajiwara, Y. Yoshimura, M. Nakano, K.
Nakajima, S. Ohira-Kawamura, T. Kikuchi, and Y. Inamura
Hyperfine structure of magnetic excitations in a Tb-based single-

MLF Operations in 2013

molecule magnet studied by high-resolution neutron spectroscopy
Physical Review B 88 64405 (2013)
56

K. Kojima
PSI 流 µSR データ解析ツール “musrfit”
日本中間子科学会 めそん 38 37 (2013)

57

K. Komatsu, M. Moriyama, T. Koizumi, K. Nakayama, H. Kagi, J.
Abe, and S. Harjo
Development of a new P–T controlling system for neutronscattering experiments
High Pressure Research 33 208 (2013)

58

S. Kubota, D. Naito, Y. Tomota, S. Harjo, C. Iio, and S. Yamaguch
Effect of Microstructure on Mechanical Properties andMachinability of Spheroidal Graphite Cast Iron
球状黒鉛鋳鉄の機械的性質と切削性に及ぼすミクロ組織の影響
Journal of Japan Foundry Engineering Society/ 鋳造工学 85 489(2013)

59

M. Kureta, A. Ohzu, M. Haruyama, M. Takase, N. Kurata, N.
Kobayashi, K. Soyama, T. Nakamura, H. Nakamura, and M. Seya
Design of an Alternative Plutonium Canister Assay system (APCA)
using ceramic scintillator neutron detectors for the safeguards
NDA
Proceedings of the 54th INMM Annual Meeting #176 (2013)

60

K. Kusaka, T. Hosoya, T. Yamada, K. Tomoyori, T. Ohhara, M.
Katagiri, K. Kurihara, I. Tanaka, and N. Niimura
Evaluation of performance for IBARAKI biological crystal
diffractometer iBIX with new detectors
Journal of Synchrotron Radiation 20 994 (2013)

61

T. Kusano, H. Iwase, K. Akutsu, T. Yoshimura, and M. Shibayama
Structural Study of Organic Salts Effect on the Trimeric Surfactant
Aggregates
構造学的視点から観た三鎖界面活性剤会合体への塩効果の考察
Photon Factory News 31 9 (2013)

62

K. D. Litasov, I. S. Sharygin, P. I. Dorogokupets, A. Shatskiy, P. N.
Gavryushkin, T. S. Sokolova, E. Ohtani, J. Li, and K. Funakoshi
Thermal equation of state and thermodynamic properties of ironcarbide Fe3C to 31 GPa and 1473 K
Journal of Geophysical Research: Solid Earth 118 5274 (2013)

63

K. D. Litasov, A. Shatskiy, P. N. Gavryushkin, I. S. Sharygin,
P. I. Dorogokupets, A. M. Dymshits, E. Ohtani, Y. Higo, and K.
Funakoshi
P–V–T equation of state of siderite to 33 GPa and 1673 K
Physics of the Earth and Planetary Interiors 224 83 (2013)

64

Z. L. Mahyari, A. Cannell, E. V. L. de Mello, M. Ishikado, H.
Eisaki, R. Liang, D. A. Bonn, and J. E. Sonier
Universal inhomogeneous magnetic-field response in the normal
state of cuprate high-Tc superconductors
Physical Review B 88 144504 (2013)

65

M. Martin, and S. Jun
Muon-spin relaxation study on Li- and Na-diffusion in solids
Physica Scripta 88 68509 (2013)

66

G. Matsuba, M. Sakurai, T. Tominaga, and S. Takata
Shish-kebab formation process observation using new SANS
spectrometer TAIKAN
Proceedings of The 12th Asian Textile Conference 55 (2013)

67

K. Matsuda, T. Nagao, Y. Kajihara, M. Inui, K. Tamura, J.
Nakamura, K. Kimura, M. Yao, M. Itou, Y. Sakurai, and N.

Sound velocity measurements in liquid Fe–S at high pressure:
Implications for Earth's and lunar cores
Earth and Planetary Science Letters 362 182 (2013)

HiraokaElectron momentum density in liquid silicon
Physical Review B 88 115125 (2013)
68

M. Medarde, M. Mena, J. L. Gavilano, E. Pomjakushina, J.
Sugiyama, K. Kamazawa, V. Y. Pomjakushin, D. Sheptyakov, B.
Batlogg, H. R. Ott, M. Månsson, and F. Juranyi
1D to 2D Na Ion Diffusion Inherently Linked to Structural
Transitions in Na0.7CoO2
Physical Review Letters 110 266401 (2013)

69

S. Meigo, M. Ooi, A. Akutsu, K. Ikezaki, H. Fujimori
Development of beam flattening system using non-linear beam
optics at J-PARC
Proceedings of International Topical Meeting on Nuclear
Applications of Accelerators TUPAT06 (2013)70

S. Meigo, M. Ooi, K. Ikezaki, A. Akutsu, S. Sakamoto, M.
Futakawa
Development of profile monitor system for high intense spallation
neutron source
Proceedings of International Beam Instrumentaion Conference,
IBIC2012 MOPB68 (2013)

71

K. Mitamura, N. L. Yamada, H. Sagehashi, N. Torikai, H. Arita, M.
Terada, M. Kobayashi, S. Sato, H. Seto, S. Goko, M. Furusaka, T.
Oda, M. Hino, H. Jinnai, and A. Takahara
Novel neutron reflectometer SOFIA at J-PARC/MLF for in-situ
soft-interface characterization
Polymer Journal 45 100 (2013)72

Y. Miyake, Y. Ikedo, K. Shimomura, P. Strasser, N. Kawamura, K.
Nishiyama, A. Koda, H. Fujimori, S. Makimura, J. Nakamura, T.
Nagatomo, R. Kadono, E. Torikai, M. Iwasaki, S. Wada, N. Saito, K.
Okamura, K. Yokoyama, T. Ito, and W. Higemoto
Ultra slow muon microscopy by laser resonant ionization at
J-PARC, MUSE
Hyperﬁne Interactions 216 79 (2013)

73

K. Mukai, Y. Ikedo, K. Kamazawa, J. H. Brewer, E. J. Ansaldo, K.
H. Chow, M. Mansson, and J. Sugiyama
The gradient distribution of Ni ions in cation-disordered
Li[Ni1/2Mn3/2]O4 clarified by muon-spin rotation and relaxation(μSR)
RSC Advances 3 11634 (2013)74

D. Naito, S. Kubota, S. Harjo, and Y. Tomota
In Situ Neutron Diffraction during Tension-Compression
Deformation for Nodular Graphite Cast Irons
ISIJ International 53 1292 (2013)75

T. Nakamura, K. Toh, T. Kawasaki, K. Honda, H. Suzuki, M.
Ebine, A. Birumachi, K. Sakasai, K. Soyama, and M. Katagiri
Evaluation of angular dependence of neutron detection efficiencies
of ZnS scintillator detectors
IEEE Nuclear Science Symposium Conference Record NPO1-211(2013)

76

77

78

T. Nakamura, K. Toh, K. Sakasai, H. Suzuki, K. Soyama, M.
Kureta, A. Ohzu, M. Takase, H. Nakamura, and M. Seya
Development of a ZnS/10B2O3 ceramic scintillator neutron detector
for safeguards NDA systems
Proceedings of the 54th INMM Annual Meeting #227 (2013)
T. Naoe, and M. Futakawa
Optically observation of mercury cavitation bubble collapsingExperimental Thermal and Fluid Science 44 550 (2013)
K. Nishida, Y. Kono, H. Terasaki, S. Takahashi, M. Ishii, Y.
Shimoyama, Y. Higo, K. Funakoshi, T. Irifune, and E. Ohtani

79

Y. Noda, D. Yamaguchi, A. Putra, S. Koizumi, Y. Sakaguchi, T.
Oku, and J. Suzuki
Polarization Analysis Equipment in SANS-J-II: Study of Polymer
Electrolyte Membrane for Fuel Cell
Physics Procedia 42 46 (2013)

80

H. Nozaki, M. Harada, S. Ohta, N. H. Jalarvo, E. Mamontov, I.
Watanabe, Y. Miyake, Y. Ikedo, and J. Sugiyama
Diffusive Behavior of Li Ions in Garnet Li5+xLa3ZrxNb2−xO12 (x =0–2)
Journal of the Physical Society of Japan 82 SA004 (2013)81

H. Nozaki, M. Månsson, B. Roessli, V. Pomjakushin, K.
Kamazawa, Y. Ikedo, H. E. Fischer, T. C. Hansen, H. Yoshida, Z.
Hiroi, and J. Sugiyama
Magnetic structure of the metallic triangular antiferromagnet
Ag2NiO2
Journal of Physics: Condensed Matter 25 286005 (2013)82

Y. Ogata, D. Kawaguchi, N. L. Yamada, and K. Tanaka
Multistep Thickening of Nafion Thin Films in Water
ACS Macro Letters 2 856 (2013)83

S. Ogo, K. Ichikawa, T. Kishima, T. Matsumoto, H. Nakai, K.
Kusaka, and T. Ohhara
A Functional [NiFe]Hydrogenase Mimic That Catalyzes Electronand Hydride Transfer from H2
Science 339 682 (2013)

84

K. Ohishi, M. Sato, S. Kototani, S. Saiki, Y. Kobayashi, and M.
Itoh
Magnetism and superconductivity in RbxFe2−ySe2
Journal of the Korean Physical Society 62 1994 (2013)85

K. Ohoyama, T. Yokoo, S. Itoh, J. Suzuki, K. Iwasa, T. J. Sato, H.
Kira, Y. Sakaguchi, T. Ino, T. Oku, K. Tomiyasu, M. Matsuura, H.
Hiraka, M. Fujita, H. Kimura, T. Sato, J. Suzuki, H. M. Shimizu, T.
Arima, M. Takeda, K. Kaneko, M. Hino, S. Muto, H. Nojiri, C. H.
Lee, J. G. Park, and S. Choi
Basic Concepts of Polarisation Analysis for Neutron Chopper
Spectrometer POLANO at J-PARC
Journal of the Physical Society of Japan 82 SA036 (2013)

86

A. Ohzu, T. Nakamura, M. Takase, N. Kurata, M. Haruyama, M.
Kureta, K. Soyama, and M. Seya
Optical guide property of alternative He-3 neutron detectors using
solid scintillators for nuclear safeguards
IEEE Nuclear Science Symposium Conference Record NPO1-195(2013)87

T. Okuchi, M. Yoshida, Y. Ohno, N. Tomioka, N. Purevjav, T.
Osakabe, S. Harjo, J. Abe, K. Aizawa, and S. Sasaki
Pulsed neutron powder diffraction at high pressure by a capacityincreased sapphire anvil cellHigh Pressure Research 33 777 (2013)

88

T. Okuda, R. Kajimoto, M. Okawa, and T. Saitoh
Effects of Hole-Doping and Disorder on the Magnetic Statesof Delafossite CuCrO 2 Having a Spin-3/2 Antiferromagnetic
Triangular SublatticeInternational Journal of Modern Physics B 27 (2013)89

M. Ooi, K. Sakai, A. Watanabe, A. Akutsu, and S. M. Takada
UPGRADE OF J-PARC/MLF GENERAL CONTROL SYSTEM
WITH EPICS/CSS
Proceedings of ICALEPCS2013 MOPPC017 (2013)

MLF Operations in 2013

205

90

M. Ooi, M. Teshigawara, T. Kai, M. Harada, F. Maekawa, M.
Futakawa, E. Hashimoto, M. Segawa, M. Kureta, A. Tremsin, T.
Kamiyama, and Y. Kiyanagi
Neutron Resonance Imaging of a Au-In-Cd Alloy for the JSNS
Physics Procedia 43 337 (2013)

100 S. Lee, J. R. Zhang, S. Torii, S. Choi, D. Y. Cho, T. Kamiyama, J.
Yu, K. A. McEwen, and J. G. Park
L a rg e i n - p l a n e d e f o r m a t i o n o f R u O 6 o c t a h e d ro n a n dferromagnetism of bulk SrRuO3
Journal of Physics: Condensed Matter 25 465601 (2013)

91

K. Osamura, S. Machiya, Y. Tsuchiya, H. Suzuki, T. Shobu, M.
Sato, S. Harjo, K. Miyashita, Y. Wadayama, S. Ochiai, and A.
Nishimura
Thermal strain exerted on superconductive filaments in practical
Nb3Sn and Nb3Al strands
Superconductor Science and Technology 26 94001 (2013)

101 S. Sanna, P. Carretta, R. De Renzi, G. Prando, P. Bonfà, M.
Mazzani, G. Lamura, T. Shiroka, Y. Kobayashi, and M. Sato
Onset of magnetism in optimally electron-doped L Fe1−xRuxAsO1−yFy(L=La, Nd, or Sm) superconductors around x =1/4
Physical Review B 87 134518 (2013)

92

T. Otomo, K. Ikeda, H. Ohshita, and K. Suzuya
Studies of Hydrogen Storage Mechanism with High Intensity
Neutron Total Scattering
高強度中性子を用いた全散乱法による水素貯蔵機構の解明
Materia Japan/ まてりあ 52 346 (2013)

102 K. Sasaki, M. Sugano, R. Ohkubo, T. Ogitsu, N. Saito, K.
Shimomura, and A. Yamamoto
Superconducting Magnet Design for the Hyperfine Structure
Measurement of Muonium at the J-PARC
Applied Superconductivity, IEEE Transactions on 23 4500704(2013)

93

S.-W. Park, H. Mizoguchi, K. Kodama, S. Shamoto, T. Otomo, S.
Matsuishi, T. Kamiya, and H. Hosono
Magnetic Structure and Electromagnetic Properties of LnCrAsO
with a ZrCuSiAs-type Structure (Ln = La, Ce, Pr, and Nd)
Inorganic Chemistry 52 13363 (2013)

103 M. Sato, Y. Kobayashi, T. Kawamata, Y. Yasui, K. Suzuki, M. Itoh,
R. Kajimoto, K. Ikeuchi, M. Arai, and P. Bourges
On the superconducting symmetry of Fe-based systems — Impurity
effect studies and neutron scattering measurements
Journal of the Korean Physical Society 62 1726 (2013)94

J. D. Parker, M. Harada, K. Hattori, S. Iwaki, S. Kabuki, Y.
Kishimoto, H. Kubo, S. Kurosawa, Y. Matsuoka, K. Miuchi, T.
Mizumoto, H. Nishimura, T. Oku, T. Sawano, T. Shinohara, J.
Suzuki, A. Takada, T. Tanimori, and K. Ueno
Spatial resolution of a μPIC-based neutron imaging detector
Nuclear Instruments and Methods in Physics Research Section A
726 155 (2013)

104 K. Sato, M. Matsuura, M. Fujita, R. Kajimoto, S. Ji, K. Ikeuchi, M.
Nakamura, Y. Inamura, M. Arai, M. Enoki, and K. Yamada
High-energy magnetic excitations in underdoped La1.90Sr0.10CuO4
Journal of the Korean Physical Society 62 1836 (2013)

95

96

206

J. D. Parker, M. Harada, K. Hattori, S. Iwaki, S. Kabuki, Y.
Kishimoto, H. Kubo, S. Kurosawa, Y. Matsuoka, K. Miuchi, T.
Mizumoto, H. Nishimura, T. Oku, T. Sawano, T. Shinohara, J.
Suzuki, A. Takada, T. Tanimori, K. Ueno, M. Ikeno, M. Tanaka,
and T. Uchida
Development of a Time-resolved Neutron Imaging Detector Basedon the μPIC Micro-Pixel Chamber
μPIC (Micro-Pixel Chamber) を用いた中性子イメージング検出器の開発
Hamon/ 波紋 23 218 (2013)
J. D. Parker, K. Hattori, H. Fujioka, M. Harada, S. Iwaki, S.
Kabuki, Y. Kishimoto, H. Kubo, S. Kurosawa, K. Miuchi, T.
Nagae, H. Nishimura, T. Oku, T. Sawano, T. Shinohara, J. Suzuki,
A. Takada, T. Tanimori, and K. Ueno
Neutron imaging detector based on the micro-pixel chamber
Nuclear Instruments and Methods in Physics Research Section A
697 23 (2013)

97

K. Sadakane, M. Nagao, H. Endo, and H. Seto
Membrane formation by preferential solvation of ions in mixture ofwater, 3-methylpyridine, and sodium tetraphenylborate
The Journal of Chemical Physics 139 (2013)

98

T. Sakamaki, A. Suzuki, E. Ohtani, H. Terasaki, S. Urakawa, Y.
Katayama, K. Funakoshi, Y. Wang, J. W. Hernlund, and M. D.
Ballmer
Ponded melt at the boundary between the lithosphere andasthenosphere
Nature Geoscience 6 1041 (2013)

99

K. Sakasai, K. Toh, T. Nakamura, K. Takakura, C. Konno, and Y.
IwamotoApplication of KCl:Eu2+ Storage Phosphors to Wide-range Neutron
Detection
IEEE Nuclear Science Symposium Conference Record NPO1-26(2013)MLF Operations in 2013

105 M. Sato, Y. Kobayashi, T. Kawamata, Y. Yasui, K. Suzuki, M. Itoh,
R. Kajimoto, K. Ikeuchi, M. Arai, and P. Bourges
On the superconducting symmetry of Fe-based systems — Impurity
effect studies and neutron scattering measurements
Journal of the Korean Physical Society 62 1726 (2013)
106 M. Segawa, T. Kai, T. Sakai, M. Ooi, and M. Kureta
Development of a high-speed camera system for neutron imaging
at a pulsed neutron source
Nuclear Instruments and Methods in Physics Research Section A
697 77 (2013)
107 A. Shatskiy, I. S. Sharygin, P. N. Gavryushkin, K. D. Litasov, Y.
M. Borzdov, A. V. Shcherbakova, Y. Higo, K. Funakoshi, Y. N.
Palyanov, and E. Ohtani
The system K2CO3-MgCO3 at 6 GPa and 900–1450 °C
American Mineralogist 98 1593 (2013)
108 A. Shatskiy, P. N. Gavryushkin, I. S. Sharygin, K. D. Litasov, I.
N. Kupriyanov, Y. Higo, Y. M. Borzdov, K.-i. Funakoshi, Y. N.
Palyanov, and E. Ohtani
Melting and subsolidus phase relations in the system Na2CO3MgCO3±H2O at 6 GPa and the stability of Na2Mg(CO3)2 in theupper mantle
American Mineralogist 98 2172 (2013)
109 P. Strasser, Y. Ikedo, Y. Miyake, K. Shimomura, N. Kawamura,
K. Nishiyama, S. Makimura, H. Fujimori, A. Koda, J. Nakamura,
T. Nagatomo, T. Adachi, A. D. Pant, T. Ogitsu, Y. Makida, M.
Yoshida, K. Sasaki, T. Okamura, H. Ohhata, T. Nakamoto, R.
Okada, R. Ohkubo, A. Yamamoto, W. Higemoto, T. U. Itoh, K.
Ishida, and K. Nakahara
Superconducting curved transport solenoid with dipole coils forcharge selection of the muon beam
Nuclear Instruments and Methods in Physics Research Section B
317 361 (2013)
110 M. Sugano, K. Sasaki, R. Ohkubo, T. Kume, N. Kimura, R. Okada,
T. Okamura, K. Shimomura, N. Saito, T. Ogitsu, and A. Yamamoto
Cryogenic Design of a Superconducting Solenoid for Muonium

Hyperfine Structure Measurement
IEEE Transactions on Applied Superconductivity 23 3800204(2013)
111 M. Sugawara, T. Hayakawa, M. Oshima, Y. Toh, A. Osa, M.
Matsuda, T. Shizuma, Y. Hatsukawa, H. Kusakari, T. Morikawa, Z.
G. Gan, and T. Czosnyka
Possible band termination in 99Rh
Physical Review C 87 64319 (2013)
112 J. Sugiyama
Ion Diffusion in Solids Probed by Muon-Spin Spectroscopy
Journal of the Physical Society of Japan 82 SA023 (2013)
113 H. Suzuki, and S. Harjo
N e u t ro n d i f f r a c t i o n s t u d i e s o n s t r a i n - d e p e n d e n c e o fsuperconducting properties in practical superconducting composite
Neutron News 24 18 (2013)114 H. Suzuki, S. Harjo, J. Abe, P. Xu, K. Aizawa, and K. Akita
Effects of gauge volume on pseudo-strain induced in strain
measurement using time-of-flight neutron diffraction
Nuclear Instruments and Methods in Physics Research Section A
715 28 (2013)
115 S. Takahashi, E. Ohtani, H. Terasaki, Y. Ito, Y. Shibazaki, M. Ishii,
K. Funakoshi, and Y. Higo
Phase relations in the carbon-saturated C–Mg–Fe–Si–O
system and C and Si solubility in liquid Fe at high pressure andtemperature: implications for planetary interiors
Physics and Chemistry of Minerals 40 647 (2013)
116 S. Takai, Y. Doi, S. Torii, J. Zhang, T. Y. S. P. Putra, P. Miao, T.
Kamiyama, and T. Esaka
Structural and electrical properties of Pb-substituted La2Mo2O9oxide ion conductors
Solid State Ionics 238 36 (2013)
117 S. Takai, T. Esaka, and T. Kamiyama
Defect Structure and Oxide-Ion Conduction Properties of PbSubstituted La2Mo2O9
Pb を添加した La2Mo2O9 の欠陥構造と酸化物イオン伝導特性
Photon Factory News 31 27 (2013)
118 I. Tanaka, and K. Kusaka
Biomacromolecular Neutron Crystallography
Sample Preparation, Diffractometers, Measurements and Data
Reduction for Neutron Protein Crystallography
生体分子の中性子単結晶解析
タンパク質中性子結晶構造解析のための試料作成、回折計、測定およびデータ処理
Hamon/ 波紋 23 288 (2013)
119 Y. Toh, C. J. Chiara, E. A. McCutchan, W. B. Walters, R. V. F.
Janssens, M. P. Carpenter, S. Zhu, R. Broda, B. Fornal, B. P. Kay,
F. G. Kondev, W. Królas, T. Lauritsen, C. J. Lister, T. Pawłat,
D. Seweryniak, I. Stefanescu, N. J. Stone, J. Wrzesiński, K.
Higashiyama, and N. Yoshinaga
Evidence for rigid triaxial deformation at low energy in 76Ge
Physical Review C 87 41304 (2013)
120 K. Toh, T. Nakamura, K. Sakasai, K. Soyama, M. Hino, M.
Kitaguchi, and H. Yamagishi
Development of two-dimensional multiwire-type neutron detector
system with individual line readout and optical signal transmission
Nuclear Instruments and Methods in Physics Research Section A
726 169 (2013)
121 Y. Tomota, and S. Harjo
Deformation Behavior of Ferrous Materials Studied by Using

Neutron Diffraction
中性子回折を用いた鉄系材料の変形特性の解析
Journal of the JSTP/ 塑性と加工 54 891 (2013)
122 K. Tomoyori, K. Kusaka, T. Yamada, T. Hosoya, T. Ohhara, K.
Kurihara, I. Tanaka, M. Katagiri, and N. Niimura
Profile functions to reproduce Bragg reflection shapes observed bya time-of-flight single-crystal diffractometer installed at a coupledmoderator pulsed neutron source in J-PARC
Nuclear Instruments and Methods in Physics Research Section A
723 128 (2013)
123 N. Tsujino, Y. Nishihara, Y. Nakajima, E. Takahashi, K.-i.
Funakoshi, and Y. Higo
Equation of state of γ-Fe: Reference density for planetary cores
Earth and Planetary Science Letters 375 244 (2013)
124 T. Wakui, H. Ishii, T. Naoe, T. Wan, X. Zhihong, K. Haga, H.
Takada, and M. Futakawa
Investigation on HIP diffusion bonding of invar ally to stainlesssteel
Proceedings of IJST2013 85 (2013)
125 T. Wan, T. Wakui, T. Naoe, M. Futakawa, K. Kawashima, and K.
Maekawa
Pitting damage imaging by non-linear ultrasonic technique:comparison between resonance and non-resonance modes
International Journal of Materials and Product Technology 46 141(2013)
126 T. Wan, T. Wakui, T. Naoe, M. Futakawa, and K. Maekawa
A Novel Ultrasonic Evaluation Process for Cavitation Damage by
Combination of Attenuation and Higher Harmonics
Journal of JSEM/ 実験力学 13 387 (2013)
127 H. Wang, C. Yang, J. Lu, M. Wu, J. Su, K. Li, J. Zhang, G. Li, T.
Jin, T. Kamiyama, F. Liao, J. Lin, and Y. Wu
On the Structure of α-BiFeO3
Inorganic Chemistry 52 2388 (2013)
128 R. Wang, C. Yang, M. Fan, M. Wu, C. Wang, X. Yu, J. Zhu, J.
Zhang, G. Li, Q. Huang, D. Chen, T. Jin, T. Kamiyama, F. Liao,and J. Lin
Phase relationship of the TbO1.81–Mn3O4–Fe2O3 system synthesized
at 1200°C
Journal of Alloys and Compounds 554 385 (2013)
129 A. Watanabe, K. Sakai, M. Ooi, S. Meigo, and H. Takada
Upgrade of general control system employed for Materials andLife Science Experimental Facility of J-PARC
J-PARC 物質・生命科学実験施設の全体制御システムのアッ
プグレード
JAEA-Technology 2013-028 (2013)
130 T. Xia, H. Ogawa, R. Inoue, K. Nishida, N. L. Yamada, G. Li, and T.
KanayaDewetting Process of Deuterated Polystyrene and Poly(vinyl
methyl ether) Blend Thin Films via Phase Separation
Macromolecules 46 4540 (2013)
131 N. Yabuuchi, Y. Kawamoto, R. Hara, T. Ishigaki, A. Hoshikawa, M.
Yonemura, T. Kamiyama, and S. Komaba
A Comparative Study of LiCoO 2 Polymorphs: Structural andElectrochemical Characterization of O2-, O3-, and O4-type Phases
Inorganic Chemistry 52 9131 (2013)132 T. Yamada, T. Yamada, M. Tyagi, M. Nagao, H. Kitagawa, and O.
Yamamuro
Phase Transition and Dynamics of Water Confined in Hydroxyethyl
Copper Rubeanate Hydrate

MLF Operations in 2013

207

Journal of the Physical Society of Japan 82 SA010 (2013)
133 S. Yano, S. Itoh, T. Yokoo, S. Satoh, D. Kawana, Y. Kousaka, J.
Akimitsu, and Y. Endoh
Magnetic excitations in ferromagnetic phase of MnPJournal of Magnetism and Magnetic Materials 347 33 (2013)
134 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, and S. Muto
Newly Proposed Inelastic Neutron Spectrometer POLANO
Journal of the Physical Society of Japan 82 SA035 (2013)
135 T. Yokoyama, M. Mizuguchi, and K. Kusaka
Hydrogen-bond Network and pH Sensitivity in Transthyretin
トランスサイレチンにおける水素結合ネットワークと pH 感
受性
Hamon/ 波紋 23 142 (2013)
136 T. Yokoyama, M. Mizuguchi, Y. Nabeshima, K. Kusaka, T.
Yamada, T. Hosoya, T. Ohhara, K. Kurihara, I. Tanaka, and N.
Niimura208

MLF Operations in 2013

Hydrogen-bond network and pH sensitivity in human transthyretin
Journal of Synchrotron Radiation 20 834 (2013)
137 M. Yonemura
BL09“Special Environment Neutron Powder Diffractometer(SPICA)”
BL09「特殊環境中性子回折装置（SPICA）」
SHIKI (Industrial Users Society for Neutron Application) / 中性子
産業利用推進協議会季報「四季」19 2 (2013)
138 T. Yoshiie, M. Futakawa, T. Naoe, M. Komatsu, K. Sato, Q. Xu,
and M. Kawai
Pitting Damage in Metals by Mercury Cavitation with MIMTM
MIMTM を用いた水銀キャビテーションによる金属の壊食損
傷構造
Materia Japan/ まてりあ 52 390 (2013)
139 J. Zhu, W. Han, J. Zhang, H. Xu, S. C. Vogel, C. Jin, F. Izumi, K.
Momma, Y. Kawamura, and Y. Zhao
Nuclear and charge density distributions in ferroelectric PbTiO3:
maximum entropy method analysis of neutron and X-ray diffraction
data
Powder Diffraction 28 276 (2013)

Editorial Board - MLF Annual Report 2013

Chief Editor

Kaoru Sakasai
Neutron Instrumentation Section

Shin-ichiro Meigo
Neutron Source Section

Takashi Wakui

Mitsutaka Nakamura

Neutron Source Section

Neutron Science Section

Takashi Ino

Kaoru Shibata

Neutron Science Section

Neutron Science Section

Kenji M. Kojima

Naritoshi Kawamura

Muon Science Section

Muon Science Section

Toshiki Asai

Garry ForanCROSS-TokaiCROSS-Tokai

Taketo Moyoshi

Hiroshi Kira

CROSS-TokaiCROSS-Tokai

MLF 2013

209

MLF Annual Report 2013

J-PARC 14-03
KEK Progress Report 2014-4

Materials and Life Science Division
J-PARC Center

Tokai, Naka-gun, Ibaraki 319-1195, Japan

http://j-parc.jp/MatLife/en/index.html

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