JAEA-Review

研究炉（JRR-3及びJRR-4）
利用における研究成果集（平成１９年度）
Activity Report on the Utilization of Research Reactors (JRR-3 and JRR-4)(Japanese Fiscal Year, 2007)（編）研究炉利用課(Ed.) Research Reactor Utilization Section

東海研究開発センター
原子力科学研究所
研究炉加速器管理部
Department of Research Reactor and Tandem Accelerator
Nuclear Science Research InstituteTokai Research and Development Center

March 2012
Japan Atomic Energy Agency

日本原子力研究開発機構

JAEA-Review

2011-050

,#'#4GXKGY
⎇ⓥἹ㧔,44 ෸߮ ,44㧕೑↪ߦ߅ߌࠆ⎇ⓥᚑᨐ㓸㧔ᐔᚑ㧝㧥ᐕᐲ㧕ᣣᧄේሶജ⎇ⓥ㐿⊒ᯏ᭴᧲ᶏ⎇ⓥ㐿⊒࠮ࡦ࠲࡯ේሶജ⑼ቇ⎇ⓥᚲ ⎇ⓥἹടㅦེ▤ℂㇱ㧔✬㧕⎇ⓥἹ೑↪⺖㧔 ᐕ  ᦬  ᣣฃℂ㧕 ᐔᚑ  ᐕᐲ‫ޔ‬㕖▤ℂ඙ၞߦ߅ߌࠆᳪᨴ߇⊒⷗ߐࠇߚߎߣߦ઻߁‫ޔ‬ౣ⊒㒐ᱛߩߚ߼ߩ
቟ో⏕⹺⺞ᩏߢ  ᦬  ᣣ߆ࠄ  ᦬  ᣣ߹ߢේሶἹࠍ஗ᱛߒߚ‫ޕ‬,44 ߪ 4 ࠨࠗࠢ࡞  ᦬  ᣣ㨪 ᦬  ᣣ ࠍ቟ో⏕⹺⺞ᩏߢ஗ᱛߒߚ߇‫ޔ‬4 ࠨࠗࠢ࡞  ᦬  ᣣ㨪 ᦬  ᣣ ࠍㅊടߒ‫ޔ‬ᐕ㑆  ࠨࠗࠢ࡞ߩㆇォࠍⴕߞߚ‫ޕ‬,44 ߪᐕ㑆ㆇォ੍ቯࠨࠗࠢ࡞߇  ࠨࠗࠢ࡞ߢ޽ߞߚ߇‫ޔ‬቟ో⏕⹺⺞ᩏ‫ޔ‬෻኿૕ⷐ⚛
⇣Ᏹߦ઻߁஗ᱛߦࠃࠅᐕ㑆  ࠨࠗࠢ࡞ߩㆇォࠍⴕߞߚ‫ޕ‬,44 ߪ‫ޔ‬ਛᕈሶᢔੂ‫ޔ‬හ⊒ࠟࡦࡑ✢ಽᨆ‫ޔ‬ਛᕈሶ࡜ࠫࠝࠣ࡜ࡈࠖߥߤߩታ㛎೑↪෸߮‫ޔ‬᡼኿ൻಽᨆ‫ޔ‬ේሶἹΆᢱ᧚ᢱ‫⵾ࡊ࡯࠻࠰ࠗࠕࠝࠫ࡜ޔ‬ㅧ‫ࠢ࠶࡜࠻ࡦ࡚ࠪ࠶ࠖࡈޔ‬ᐕઍ᷹ቯߩᾖ኿೑↪╬‫ޔ‬᭽‫ߦ⊛⋡ߥޘ‬೑↪ߐࠇߡ޿ࠆ‫ޕ‬,44 ߦߟ޿ߡߪ‫ޔ‬ක≮ᾖ኿㧔$QTQP0GWVTQP%CRVWTG6JGTCR[㧦$0%6㧕‫ޔ‬හ⊒ࠟࡦࡑ✢ಽᨆ‫ޔ‬᡼኿✢᷹ቯེߩᗵᐲ⹜㛎‫ޔ‬ේሶἹ⎇ୃㆇォታ⠌╬ߩታ㛎೑↪‫ޔ‬෸߮᡼኿ൻಽᨆ‫ޔ‬࡜ࠫࠝࠕࠗ࠰࠻࡯ࡊ⵾ㅧ‫ࠢ࠶࡜࠻ࡦ࡚ࠪ࠶ࠖࡈޔ‬ᐕઍ᷹ቯߩߚ߼ߩᾖ኿೑↪╬‫ޔ‬᭽‫ߥޘ‬⋡⊛ߦ೑↪ߐࠇߡ޿ࠆ‫ޕ‬ ᧄႎ๔ᦠߪ‫⎇ޔ‬ⓥἹߩ೑↪⠪㧔ේሶജᯏ᭴ᄖࠍ฽߻㧕߆ࠄᚑᨐߩឭ಴ࠍฃߌ‫ޔ‬ਛᕈሶᢔੂ  ಽ㊁㧔᭴ㅧ‫⏛ޔ‬ᕈ‫⿥ޔ‬વዉߥߤ㧕‫ޔ‬ਛᕈሶ࡜ࠫࠝࠣ࡜ࡈࠖ‫ޔ‬හ⊒ࠟࡦࡑ✢ಽᨆ‫ޔ‬᡼኿ൻಽᨆ‫ߩޔઁߩߘޔ‬ಽ㊁೎ߦ⎇ⓥᚑᨐࠍขࠅ߹ߣ߼ߚ߽ߩߢ޽ࠆ‫ޕ‬






ේሶജ⑼ቇ⎇ⓥᚲ㧦‫⨙ ޥ‬ၔ⋵㇊⃗㇭᧲ᶏ᧛⊕ᣇ⊕ᩮ 㫀㩷
JAEA-Review 2011-050
Activity Report on the Utilization of Research Reactors (JRR-3 and JRR-4)(Japanese Fiscal Year, 2007)(Ed.) Research Reactor Utilization Section
Department of Research Reactor and Tandem Accelerator
Nuclear Science Research InstituteTokai Research and Development Center
Japan Atomic Energy Agency
Tokai-mura, Naka-gun, Ibaraki-ken(Received Decemder 16, 2011)
In the fiscal year 2007, the research reactor JRR-3 was operated for 7 cycles (cycle operation :26days/cycle) and the JRR-4㩷 was operated for 92 days.
JRR-3 is used for the purposes below;- Experimental studies such as neutron scattering, prompt gamma-ray analyses,
neutron radiography- Irradiation for activation analyses, radioisotope (RI) productions, fission tracks- Irradiation test of reactor materialsetc.
JRR-4 is used for the purposes below;- Medical irradiation (Boron Neutron Capture㩷 Therapy : BNCT)- Prompt gamma-ray analyses- Sensitivity measurement of radiation detectors- Experiment and practice in the nuclear reactor training- Irradiation for activation analyses, RI productions, fission tracks
etc.
The volume contains 262activity reports, which are categorized into the fields of neutron
scattering (10㩷 subcategories), neutron radiography, neutron activation analyses, prompt
gamma-ray analyses, and others submitted by the users in JAEA and other Organizations.
Keywords: JRR-3, JRR-4, Research Reactor, Neutron Scattering, Neutron Radiography,
Neutron Activation Analysis, Neutron Beam, Irradiation

㫀㫀㩷JAEA-Review 2011-050┠

ḟࡣࡌࡵ࡟ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐

1◊✲ᡂᯝ୍ぴ3͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐
1. ୰ᛶᏊᩓ஘ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐
1) ᵓ㐀࣭ບ☢ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐
2) ☢

21
21

ᛶ

95
͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐3) ᙉ┦㛵㟁Ꮚ⣔ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 1654) 㠀ᬗ㉁㺃ᾮయ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 2115) 㧗ศᏊ

͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐

2256) ⏕≀ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 261
7) ᇶ♏≀⌮Ꮫ㺃୰ᛶᏊගᏛ
279
͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐
8) ⿦⨨ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 2879) ㉸ఏᑟ⌧㇟͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 309
10) ṧ␃ᛂຊ
313
͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐
2. ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 319
3.

༶Ⓨ࣐࢞ࣥ⥺ศᯒ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐

339

4. ᨺᑕ໬ศᯒ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 347
5. ࡑࡢ௚ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 377
࠾ࢃࡾ࡟398͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐
ㅰ ㎡ ͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐ 399
௜ 㘓͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐͐Ϻ

401

JAEA-Review 2011-050

Contents

Preface ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖

1

Research Reports3̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖
1. Neutron Scattering ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖
1) Structure㨯Excitation ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖

21212) Magnetism95̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖
3) Strongly Correlated Electron Systems ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 165
4) Amorphous࡮Liquid ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 211

5) Polymer̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖

225

6) Biology ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 261
7) Fundamental Physics࡮Neutron Optics
279̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖
8) Instrument ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 287
9) Superconductivity ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 309
10) Residual Stress313̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖
2. Neutron Radiography ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 319
3. Prompt Gamma-ray Analyses̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖

339

4. Neutron Activation Analyses ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 347
5. Others ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 377
Conclusion
398̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖
Acknowledgments ̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ 399
Appendixes̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖̖ζ

401

JAEA-Review 2011-050⎇ⓥἹ೑↪ߦ߅ߌࠆ⎇ⓥᚑᨐ㓸 ᐔᚑ  ᐕᐲ ߪߓ߼ߦ ᐔᚑ㧝㧥ᐕᐲߦߪ‫ޔ‬㧶㧾㧾㧙㧟ߦ߅޿ߡ㧣ࠨࠗࠢ࡞ߩ౒ห೑↪ㆇォ‫ޔ‬㧶㧾㧾㧙㧠ߦ߅޿ߡ㧞㧡ࠨࠗࠢ࡞ߩ౒ห೑↪ㆇォ߇ⴕࠊࠇ‫ߥ߹ߑ߹ߐ޿઻ߦࠇߎޔ‬೑↪߇ⴕࠊࠇߚ‫ޕ‬ ᧄႎ๔ᦠߪ‫ޔ‬೑↪⠪㧔ේሶജᯏ᭴ᄖ೑↪⠪ࠍ฽߻㧕߆ࠄᒰ⹥೑↪ߩᚑᨐߩឭ಴ࠍฃߌ‫ޔ‬ขࠅ߹ߣ߼ߚ߽ߩߢ޽ࠆ‫ޕ‬ឭ಴ߒߡ㗂޿ߚᚑᨐߩઙᢙߪ‫ޔ‬ਛᕈሶᢔੂ㧞㧠㧜ઙ‫ޔ‬ਛᕈሶ࡜ࠫࠝࠣ࡜ࡈࠖ㧢ઙ‫ޔ‬හ⊒ࠟࡦࡑ✢ಽᨆ㧡ઙ‫ޔ‬᡼኿ൻಽᨆ㧣ઙ‫ઁߩߘޔ‬㧠ઙߢว⸘㧞㧢㧞ઙߢ޽ߞߚ‫ᧄޔ߅ߥޕ‬ႎ๔ᦠߩ৻ㇱߪ‫⾆ޔ‬㊀ߥ⎇ⓥᚑᨐࠍ౏㐿ߔࠆᯏળࠍᐢߍࠆߚ߼‫ޔ‬ਅ⸥ႎ๔ᦠߩਛ߆ࠄォタߐߖߡ㗂޿ߚ߽ߩߢ޽ࠆ‫ޕ‬ ᦨᓟߦ‫ޔ‬ේⓂࠍឭ಴ߒߡ㗂޿ߚ೑↪⠪ߩ⊝᭽ߩߏදജߦᗵ⻢ߔࠆߣߣ߽ߦ‫੹ޔ‬ᓟ߽⎇ⓥἹ߇᦭ലߦ೑↪ߐࠇ‫ޔ‬⒳‫⎇ߩޘ‬ⓥ߇ߐࠄߦㅴዷߐࠇࠆߎߣࠍᦼᓙߒ߹ߔ‫ޕ‬      ⎇ⓥἹ೑↪⺖㐳 ╣ፉ ᢥ㓶    ᮡ   㗴㧦#%6+8+6;4'2146100'764105%#66'4+0)
  4'5'#4%*KUUWGFD[+55205.7PKXGTUKV[QH6QM[Q8QN   㧔᧲੩ᄢቇ‛ᕈ⎇ⓥᚲ⊒ⴕ㧕    ✬   ⠪㧦᧲੩ᄢቇ‛ᕈ⎇ⓥᚲ    ⊒ ⴕ ᐕ㧦㧞㧜㧜㧤ᐕ    ᮡ   㗴㧦ේሶജᯏ᭴ᣉ⸳೑↪౒ห⎇ⓥᚑᨐႎ๔ᦠ㧔ᐔᚑ㧝㧥ᐕᐲ㧕    ✬   ⠪㧦᧲੩ᄢቇᄢቇ㒮Ꮏቇ♽⎇ⓥ⑼ේሶജኾ᡹౒ห೑↪▤ℂᧄㇱ ⊒ ⴕ ᐕ㧦㧞㧜㧜㧤ᐕ㻙㻌 㻝㻌㻙This is a blank page.

JAEA-Review 2011-050
















⎇ ⓥ ᚑ ᨐ ৻ ⷩResearch Reports㻙㻌 㻟㻌㻙This is a blank page.

JAEA-Review 2011-050

No.
㪈㪄㪈㪄㪈
㪈㪄㪈㪄㪉
㪈㪄㪈㪄㪊
㪈㪄㪈㪄㪋

㪈㪄㪈㪄㪌
㪈㪄㪈㪄㪍

㪈㪄㪈㪄㪎

㪈㪄㪈㪄㪏
㪈㪄㪈㪄㪐

㪈㪄㪈㪄㪈㪇
㪈㪄㪈㪄㪈㪈
㪈㪄㪈㪄㪈㪉
㪈㪄㪈㪄㪈㪊
㪈㪄㪈㪄㪈㪋
㪈㪄㪈㪄㪈㪌
㪈㪄㪈㪄㪈㪍
㪈㪄㪈㪄㪈㪎
㪈㪄㪈㪄㪈㪏
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㪈㪄㪈㪄㪉㪇

䇸䇭T i t l e䇭䇹
Neutron Scattering - Structure 䊶 Excitation Correlation between structural and thermoelectric properties in Zn13Sb10
G. Nakamoto, A. Tada, M. Kurisu, A. Tanaka, T. Tsutaoaka, Y. AndohDynamics of the water included in [H11O5][ZnCu(CN)4]
S. Nishikiori, Y. Minamimoto, O. Yamamuro
Structural phase transition of one-dimensional semiconductor C5H10NH2PbI3
M. Takahashi, K. Kawasaki, K. Kataoka, Y. Fujii, M.Watanabe, K. Ohshima, Y. Noda
Superspace Group Approach to the Crystal Structure of Chimney-LadderCompound [Mn][Si]gY. Miyazaki, D. Igarashi, T. Kajitani
Structure analysis of trehalose dihydrate by neutron diffraction
M. Takahashi, K. Kawasaki, K. Kataoka, M.Watanabe, K. Ohshima, Y. Noda
QENS studies of Fast Molecular Reorientation in Liquid, Glass and Crystalline
Phases of 8*OCB
H. Suzuki, A. Inaba, J. Krawczyk, M. Massalska-Arodz, T. Kikuchi, O. Yamamuro
Crystal Structure of Tantalum Oxynitride TaON, a Visible Light Responsive
Photocatalyst
M. Yashima, Y. Lee, K. Domen
Diffusion Path of Oxide Ions in Apatite-type La9.25Si6.0O25.88
R. Ali, M. Yashima, Y. Matsushita, F. Izumi, S.Kikkawa, T. Wakita
Structural investigation of the cubic perovskite-type doped lanthanum cobaltite
La0.6Sr0.4CoO3-delta at 1258 degrees Celsius, - Possible diffusion path of oxygenions in an electrode material
M. Yashima, T. Tsuji
Low-Energy Phonon Anomaly of CeOs4Sb12
K. Iwasa, S. Itobe, C. Yang, Y. Murakami, M. Kohgi, H. Sugawara, H. Sato
Observation of spin dynamics in Shastry- Shutherland lattice TbB4
K. Ohoyama, T. Matsumura, D. Okuyama, F. Iga, S. Michimura
Crystal Structure of Chemically Modified Layered Cobaltates
Y. Miyazaki, D. Igarashi, T. Kajitani
Structural disorder of cubic Ce0.5Zr0.5O2 solid solution
T. Wakita, M. Yashima, Y. Matsushita, T.Komatsu, Yong Phat, T. Ohta
Magnetic structure in CuFeP66
M. Takahashi, E. Ahmed, K. Ohshima, Y. Noda
Magnetic excitation in CuFeP66
M. Takahashi, E. Ahmed, K. Ohshima, N. Matsura
Neutron scattering study of phonon dynamics on La3Pd20Ge6
C. H. Lee, H. Yoshizawa, I. Hase, Y. Nemoto, T. Goto
Lattice dynamics of NaNbO3
I. Tomeno, Y. Tsunoda, M. Nishi, M. Matsuura, K. Oka
Crystal Structure of Mg-doped apatite-type Ionic Conductor
Y. Matsushita, T. Wakita, H. Yoshioka, M. Yashima, F. Izumi
Crystal structure and ionic conductivity of Ga system oxides for solid
electrolyte of fuel cellY. Idemoto, T. Sugiyama, N. Kitamura
Structural evaluation of nanotube and nanosheet layered titanate with novel
nanostructures by neutron diffraction method
T. Kubo, M. Yashima, A. Nakahira㪄㩷 㪌㩷㪄

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JAEA-Review 2011-050

㪈㪄㪈㪄㪉㪈 Neutron Critical Diffuse Scattering of Quantum Relaxor KTaO3:Li
H. Yokota, Y. Uesu㪈㪄㪈㪄㪉㪉 Dependence of crystal structure and ferroelectric property on compositionand heat treatment for (Pb,Si)(Zr,Ti,Nb)O3 ferroelectric material
Y. Idemoto, S. Komiya㪈㪄㪈㪄㪉㪊 Structural Defect and Ionic Conduction of Hydroxyapatite
H. Fujimori, K. Okanishi, K. Ohoyama, M. Yashima㪈㪄㪈㪄㪉㪋 Neutron diffraction study on SnO2-CeO2 system
K. Nomura, H. Kageyama, T. Maekawa, C. Minagoshi, S. Nakamura , T. Ito㪈㪄㪈㪄㪉㪌 Magnetic Phase Transition and Electric Polarization Flop of TmMn2O5
M. Fukunaga, K. Nishihata, H. Kimura, Y. Noda, K. Kohn㪈㪄㪈㪄㪉㪍 Split-hydrogen sites in trioctahedral micas
K. Ishida, H. Fukazawa
㪈㪄㪈㪄㪉㪎 Powder Neutron Diffraction Measurements of One-dimensional Magnets
MPb4Sb6S14 (M = Fe, Mn)
Y. Matsushita, M. Nishi, S. Watanabe
Crystal Structure of La-Ge-O Ionic Conductor㪈㪄㪈㪄㪉㪏
Y. Matsushita, N. Tsujii, K. Kobayashi, F. Izumi
Low energy excitation in DyB6
㪈㪄㪈㪄㪉㪐
K. Tomiyasu, K. Takahashi
High resorution inelastic neutron scattering by TiNi(Fe) alloy㪈㪄㪈㪄㪊㪇
T. Ohba, D. Kitanosono, T. Fukuda㪈㪄㪈㪄㪊㪈 Crystal Structure Analysis of a Supramolecular Ferroelectric 55DMBP-H2ia
R. Kumai, D. Okuyama, S. Horiuchi, T. Arima, M.Watanabe, Y.Noda, Y. Tokura㪈㪄㪈㪄㪊㪉 Study suggests the existence of ferroelectric ice layer on a cold planet
H. Fukazawa, H. Yamauchi, A. Hoshikawa
㪈㪄㪈㪄㪊㪊 Structures and Phase Transitions in A2BO4-type Dielectrics
H. Shigematsu, K. Nomura㪈㪄㪈㪄㪊㪋 Magnetic structure of Ni-Mn-Z(Z=In, Sn) shape memory alloys
T. Kanomata, K. Fukushima, Y. Yamaguchi㪈㪄㪈㪄㪊㪌 Crystal Structure Determination of Ba2MgSiO7 by Neutron Diffraction
S. Seki, A. Komeno, K. Uematsu, K. Toda, M. Sato㪈㪄㪈㪄㪊㪍 Diffuse Scattering Measurement on Protonic Conductor K3H(SeO4)2
F. Shikanai, S. Itoh, K. Tomiyasu, N. Aso, S. Ikeda, T. Kamiyama㪈㪄㪈㪄㪊㪎 Structural investigation of the cubic perovskite-type doped lanthanum cobaltite
La0.4Ba0.6CoO3-x
T. Ohta, M. Yashima, T. Wakita, Y. Matsushita, T. Komatsu, Y. Phat㪈㪄㪈㪄㪊㪏 Structural analysis of metavanadate phosphors AVO3 (A: K, Rb and Cs)
T. Nakajima, M. Isobe, T. Tsuchiya, Y. Ueda, T. Kumagai
Crystal structural change of potassium titanyl phosphate㪈㪄㪈㪄㪊㪐
T. Komatsu, M. Yashima, T. Wakita, Y. Phat, Y.Matsushita
Li ion distributions of layered-structure type oxides LiNi1/2Mn1/2O2 prepared by㪈㪄㪈㪄㪋㪇 ion-exchange
Y. Arachi, H. Maeda, H. Kobayashi, T. AsaiHigh temperature neutron diffraction study of (La0.9Sr0.1)MnO3+d perovskite㪈㪄㪈㪄㪋㪈 K. Nomura, H. Kageyama, K. Kakinuma, T. Maekawa, S. Nakamura, H. Miyazaki
H. Imabayashi, T. Ito
Lithium Diffusion in LixFePO4
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A.Yamada, S. Nishimura, G. Kobayashi, M. Yashima, K. Ohoyama, Y. Yamaguchi㪄㩷 㪍㩷㪄

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JAEA-Review 2011-050

㪈㪄㪈㪄㪋㪊 Soft modes in the relaxor ferroelectric compound (Na0.5Bi0.5)TiO3
M. Matsuura, H. Iida, K. Hirota, Y. Noguchi, M. Miyayama
Anisotropic damping of transverse acoustic and optical modes in the relaxor㪈㪄㪈㪄㪋㪋 ferroelectric 0.7 Pb(Mg1/3Nb2/3)O3-0.3 PbTiO3
M. Matsuura, K. Hirota
㪈㪄㪈㪄㪋㪌 Behavior of Thermal Parameters through Phase Transition in KDP
H. Mashiyama, T. Miyoshi, T. Asahi, H. Kasano㪈㪄㪈㪄㪋㪍 Crystal Structure Analysis of Ferroelectric Niobium Oxides
N. Kumada, Y. Yonesaki, T. Takei, N. Kinomura, M. Yashima㪈㪄㪈㪄㪋㪎 Water Density Near Surface of DLC Films Having Various Surface Energies
Measured by Neutron Reflectometry
T. Hirayama, T. Uno, T. Torii, T. Matsuoka, K. Inoue, T. Ebisawa, S. Tasaki, M. Hino
N. Torikai㪈㪄㪈㪄㪋㪏 Water Density Near Surface of DLC Films Having Various Surface Energies
Measured by Neutron Reflectometry
T. Hirayama, T. Uno, T. Torii, T. Matsuoka, K. Inoue, T. Ebisawa, S. Tasaki, M. Hino
N. Torikai㪈㪄㪈㪄㪋㪐 Magnetic structure of Pr2-2xCa1+2xMn2O7(x=0.45)
Y. Tokunaga, D. Okuyama, T.J. Sato, T. Arima, Y. Tokura㪈㪄㪈㪄㪌㪇 Neutron scattering in Ising-like one dimensional antiferromagnet BaCo2V2O8
T. Masuda, S. Hondo, M. Matsuura
Crystal structural analysis of rutile-type titania㪈㪄㪈㪄㪌㪈
Y. Phat, M. Yashima, T. Wakita, T. Komatsu
Diffuse Scattering of PbF2
㪈㪄㪈㪄㪌㪉
Xianglian, K. Basar, S. Siagian, T. Sakuma, H. Takahashi, N. Igawa
Structural Features of Lithium Ion Conductor Li1+x Ge2-x Alx (PO4)3
㪈㪄㪈㪄㪌㪊
Y. Fujita, H. Takahashi, T. Sakuma, N. Igawa
Xe Motion in Clathrate Deuterohydrate Analyzed by Applying㪈㪄㪈㪄㪌㪋 Rietveld/Maximum Entropy Method
N. Igawa, T. Taguchi, H. Fukazawa, H. Yamauchi, W. Utsumi, Y. Ishii
Neutron Powder Diffraction and Difference MEM Analysis of㪈㪄㪈㪄㪌㪌 Protium- and Deuterium-Dissolved BaSn0.5In0.5O2.75+a
T. Nagasaki, S. Shiotani, M. Yoshino, K. Iwasaki, N. Igawa, H. Fukazawa, W. Utsumi
㪈㪄㪈㪄㪌㪍 In Situ Powder Neutron Diffraction Experiment under High Pressure
W.Utsumi, K.Komatsu, H.Arima, H.Kagi, T.Okuchi, S.Sasaki, H.Yamauchi
H.Fukazawa, N.Igawa, T.Kamiyama㪈㪄㪈㪄㪌㪎 Pressure-Temperature Phase Diagram of Filled Skutterudite PrFe4P12
T. Osakabe, K. Kuwahara㪈㪄㪈㪄㪌㪏 Cu Dimer Excitations in Cu2Fe2Ge4O13
T. Masuda, K. Kakurai㪈㪄㪈㪄㪌㪐 Local Lattice Distortion in Giant Negative Thermal Expansion Material
Mn3Cu1-x Gex N
S. Iikubo, K. Kodama, K. Takenaka, H. Takagi, S. Shamoto㪈㪄㪈㪄㪍㪇 Existence of Ferroelectric Ice on Planets -a neutron studyH. Fukazawa
㪈㪄㪈㪄㪍㪈 Nano-structure Analysis of ODS Ferritic Steels for Fast Reactor Application
S. Ohtsuka, J. Suzuki, T. Kaito, S. Kim, M. Inoue, S. Obara, T. Asayama㪄㩷 㪎㩷㪄

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No.
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䇸䇭T i t l e䇭䇹
Neutron Scattering - Magnetism Neutron Inelastic Scattering of TbPd3S4
E. Matsuoka, K. Ohoyama, H. Onodera
Spin Correlations of a Simple Cubic Antiferromagnet Pt3Fe Alloy
R. Matsui, Y. Tsunoda
Elastic Diffuse Scattering of Neutrons in Fe3Pt Invar Alloys
M. Takasaka, Y. Tsunoda
Magnetic structure of the n=3 frustrated square-lattice quantum spin system(CuCl)Ca2Ta3O10
H. Kageyama, Y. Tsujimoto, A. Kitada, T.Watanabe, Y. Ajiro, K.Yoshimura
M. Nishi, K. Hirota
Neutron scattering study on (CuCl)LaTa2O7
H. Kageyama, A. Kitada, Y. Tsujimoto, Y. Ajiro, K. Yoshimura, M.Nishi
N. Matsuura, K. Hirota
Electric polarization induced by a proper helical magnetic ordering in a delafossite
multiferroic CuFe1-x Alx O2
T. Nakajima, S. Mitsuda, S. Kanetsuki, K. Tanaka, T. Fujii, N. Terada, M. Soda
M. Matsuura, K. Hirota
Electric field dependence of magnetic ordering of a delafossite multiferroic
CuFe1㺍㺍x Alx O2
T. Nakajima, S. Mitsuda, H. Kimura, Y. Noda
Effective random-field domain-state in a diluted frustrated magnet CuFe1㺍㺍x Alx O2
T. Nakajima, S. Mitsuda, H. Honma, H. TsuchidaPolarization analysis neutron scattering study of magnetic correlations in randommagnet Fe65(Ni-Mn)35
K. Motoya, Y. Muro
Magnetic excitations in the random-exchange Ising system (Fe-Zn)F2 near the
percolation threshold
K. Motoya, Y. Muro, N. Aso, D. P. Belanger
Inelastic Neutron Scattering Study on Triangular Lattice Antiferromagnet CuFeO2
T. Nozaki, K. Hayashi, T. Kajitani
Search for magnetic reflections in a heavy fermion antiferromagnet CeTe3
N. Aso, K. Deguchi, G. F. Chen, N. K. Sato, H. Yoshizawa
Magnetic structure of TbCoSn
M.Kurisu, A.Tada, G.Nakamoto, T.Tsutaoka, Y.AndohPressure induced incommensurate–commensurate magnetic phase transition in
multiferroic HoMn2O5
H. Kimura, K. Nishihata, Y. Noda, N. Aso, T. Fujiwara, Y. Uwatoko
Defect-induced short-range magnetic order in Co2(OD)3Cl
X.G. Zheng, M. Hagihala, T. Yamashita
Inelastic neutron scattering on DyB4
T. Matsumura, D. Okuyama, T. Mouri
Neutron diffraction in magnetic frustration systems with a 40T pulsed magnet
K. Ohoyama, K. Kurosawa, S. Yoshii, H. Nojiri, Y.H. Matsuda, H. Hiraka, S. Mitsuda
Magnetic structure of an antiferro-octupolar ordering compound Tb0.94Gd0.06B2C2
E. Matsuoka, Y. Sasaki, D. Usui. K. Ohoyama, H. Onodera
Magnetic structure of multipolar ordering compounds RPd3S4 (R = Ce, Pr)
E. Matsuoka, D. Usui, Y. Sasaki, K. Ohoyama, H. Onodera
Study on low-temperature phase transitions in the Ho3Al5O12
R. Morinaga, T. J. Sato, H. Kimura㪄㩷 㪏㩷㪄

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JAEA-Review 2011-050

㪈㪄㪉㪄㪉㪈 Magnetic and Crystallographic Study on R2CrS4 (R=Ho and Er)
K. Tezuka, Y. Yoshioka, S. Sato, S. Suzuki, K. Oshikane, Y. J. Shan, H. Imoto, K. Ohoyama㪈㪄㪉㪄㪉㪉 Magnetic structure study of the multi-step metamagnet CeIr3Si2
Y. Muro, K. Motoya, K. Shigeto, T. Takabatake㪈㪄㪉㪄㪉㪊 Magnetic phase diagram of the square lattice CuSb2-xTaxO6 with competinginteractions J1 and J2
M. Nishi, M. Kato, K. Hirota, K. Ohyama㪈㪄㪉㪄㪉㪋 Competing interactions in two dimensional square lattice CuSb2-xTaxO6
M. Nishi, M. Kato, K. Hirota, M. Matsuura㪈㪄㪉㪄㪉㪌 Crystal Field Excitation of TmAg2In
T. Matsumura㪈㪄㪉㪄㪉㪍 Magnetic Structure Analysis in Cr1-xMoxB2 (x = 0.15)
Y. Kousaka, E. Kaya, H. Kimura, Y. Noda, J. Akimitsu㪈㪄㪉㪄㪉㪎 Chiral Helimagnetism in CuB2O4
Y. Kousaka, E. Kaya, M. Matsuura, K. Hirota, M. Nishi, J.Akimitsu㪈㪄㪉㪄㪉㪏 Energy Range of Magnetic Excitations in Percolating Two-Dimensional
Heisenberg Antiferromagnet, Rb2Mn0.598Mg0.402F4
S. Itoh, T. J. Sato㪈㪄㪉㪄㪉㪐 Antiferromagnetic ordering of Ca3Ru2O7
Y. Yoshida, K. Iwata, N. Aso, S. Katano㪈㪄㪉㪄㪊㪇 Relationship between Magnetic Structure and Ferroelectricity of LiVCuO4
Y. Yasui, Y. Naito, K. Sato, T. Moyoshi, M. Sato, K. Kakurai㪈㪄㪉㪄㪊㪈 Magnetic Excitation Spectra of Honeycomb System Na3T2SbO6 (T=Cu, Ni, Co)
Y. Miura, Y. Yasui, T. Moyoshi, M. Sato, K. Kakurai㪈㪄㪉㪄㪊㪉 Neutron diffraction studies on a Pr7Ni3 single crystal
T. Tsutaoka, A. Tanaka, Y. Andoh, A. Tada, G. Nakamoto, M. Kurisu
㪈㪄㪉㪄㪊㪊 Neutron Diffraction Studies on Y7Rh3Dx
T. Tsutaoka, A. Tanaka, A. Tada, G. Nakamoto, M. Kurisu, Y. Andoh㪈㪄㪉㪄㪊㪋 Magnetic excitation spectrum in the frustrated triangular lattice antiferromagnet
CuFe1-xAlxO2
S. Mitsuda, T. Nakajima, S. Iwamoto, N. Terada㪈㪄㪉㪄㪊㪌 Magnetic Structure of Noncentrosymmetric heavy-Fermion Ce4Ni3Pb4
T. Onimaru, K. Shigetoh, A. Ishida, T. Takabatake㪈㪄㪉㪄㪊㪍 Crystal and magnetic structures of 12L-perovskites Ba4LnRu3O12 (Ln = Pr and Tb)
Y. Shimoda, Y. Doi, Y. Hinatsu㪈㪄㪉㪄㪊㪎 Magnetic excitations in MCr2O4 (M=Fe, Ni)
K. Tomiyasu, H. Hiraka, K. Ohoyama, K. Yamada㪈㪄㪉㪄㪊㪏 Spin Waves in MnPS. Yano, Y. Kousaka, M. Nishi, M. Matsuura, K. Hirota, J. Akimitsu㪈㪄㪉㪄㪊㪐 Magnetic structures and transitions of HoRh2Si2
T. Shigeoka, H. Shibasaki, T. Fujiwara, M. Nishi
㪈㪄㪉㪄㪋㪇 Neutron scattering study on the molecular magnet Mn6Sb2
K. Iida, T. J. Sato㪈㪄㪉㪄㪋㪈 Neutron scattering in Ba2MnGe2O7
T. Masuda, S. Kitaoka, M. Nishi㪄㩷 㪐㩷㪄

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㪈㪄㪉㪄㪋㪉 Neutron scattering in O2 adsorbed CPL-1
T. Masuda, K. Hirota
㪈㪄㪉㪄㪋㪊 Powder diffraction study on the ternary compound Ce5Ni2Si3
T. J. Sato, K. Iida, H. Kitazawa, Y. S. Kwon
㪈㪄㪉㪄㪋㪋 Studies of a quadrupolar ordering and magnetic excitations in YbAs
A. Oyamada, K. Kuwahara, K. Iwasa, K. Ohoyama, M. Kohgi
㪈㪄㪉㪄㪋㪌 Magnetic property of Ag-In-Tb 1/1 approximant and its relation to Zn-Mg-RE
quasicrystals
S. Ibuka, K. Iida, T. J. Sato㪈㪄㪉㪄㪋㪍 Crystal Structure and Magnetic Properties of CoZn(TeO3)Br2
T. Kashi, Y. Yasui, T. Moyoshi, M. Sato, K. Kakurai, S. Iikubo, N. Igawa㪈㪄㪉㪄㪋㪎 Linear Relation between Electric Polarization and Magnetic Chirality in theCommensurate Phase of RMn2O5 (R =Ho, Er)
S. Wakimoto, H. Kimura, M. Fukunaga, K. Nishihata, M. Takeda, K. Kakurai, Y. Noda
Y. Tokura㪈㪄㪉㪄㪋㪏 Polarization of the Spin-Wave Modes in the Kagome' Lattice Antiferromagnet
KFe3(OH)6(SO4)2
K. Matan, J. S. Helton, D. Grohol, D. G. Nocera, S. Wakimoto, K. Kakurai, Y. S. Lee㪈㪄㪉㪄㪋㪐 Investigation of in-plane Magnetic Structure in NpFeGa5
T. Sugai, F. Mizuno, K. Kaneko, N. Metoki㪈㪄㪉㪄㪌㪇 Unusual field-induced Antiferromagnetic Order in NpIn3
F. Mizuno, T. Sugai, N. Metoki, K. Kaneko㪈㪄㪉㪄㪌㪈 Magnetic Structure of LiCu2O2
Y. Yasui, K. Sato, T. Moyoshi, M. Sato, K. Kakurai㪈㪄㪉㪄㪌㪉 Investigation of the Giant Magnetic Moments in Nitrogen-Martensites thin
Films Using the Polarized Neutron Diffraction Technique
M. Takeda, K. Kakurai, K. Sunaga, M. Tsunoda, M. Takahashi㪈㪄㪉㪄㪌㪊 Partial Disordered Phase of RbCoBr3
Y. Nishiwaki, A. Oosawa, K. Kakurai, T. Kato㪈㪄㪉㪄㪌㪋 Neutron Diffraction Study on Spinel GeCo2O4 under Magnetic Field
M. Matsuda, T. Hoshi, H. A. Katori, M. Kosaka, H. Takagi㪈㪄㪉㪄㪌㪌 Magnetic Excitation in the Spin-1/2 Antiferromagnetic Alternating Chain
Compound β -AgCuPO4
M. Hase, M. Matsuda, K. Kakurai, K. Ozawa, H. Kitazawa,..
N. Tsujii, A. Donni, H. Kuore㪈㪄㪉㪄㪌㪍 Multi-step Magnetic Transition in Non-centrosymmetric Compound CeCoGe3
K. Kaneko, N. Metoki, T. D. Matsuda, A.Thamizhavel, T. Takeuchi
Y. Haga, R. Settai, Y. Onuki㪈㪄㪉㪄㪌㪎 Pressure-Induced Magnetic Quantum Phase Transition in Coupled
Spin Dimer System KCuCl3
T. Ono, J. Kawakami, H. Tanaka, T. Osakabe, K. Kakurai㪈㪄㪉㪄㪌㪏 Magnetic Structural Analysis of Magnetic Multilayers by Complementary
Use of X-ray and Neutrons
M. Takeda, D. Yamazaki, K. Soyama, R. Maruyama, M. Hino, T. Hirano㪈㪄㪉㪄㪌㪐 Small-Angle Neutron Scattering Measurements of Averaged Internal
Structures in Nd-Fe-11B Sintered Magnets
M. Takeda, J. Suzuki, D. Yamaguchi, T. Akiya, H. Kato, M. Sagawa, K. Koyama㪄㩷 㪈㪇㩷㪄

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䇸䇭T i t l e䇭䇹
Neutron Scattering - Strongly Correlated Electron SystemsMagnetic excitations in halogen-bridged nickel complex
S. Itoh, K. Nakajima
Charge and magnetic order in 2d cobaltate Pr2-xCaxCoO4
H. Yoshizawa, K. Masuda
Variation of magnetic modulation for the antiferromagnetic states in
CeRh1㺍㺍x Cox In5(x = 0, 0.5 and ~ 0.7)
N. Oyama, M. Yokoyama, S. Oinuma, I. Kawasaki, H. Amitsuka, K. Tenya
T. J. Sato, M. Matsuura, K. Hirota
Evolution of Ferromagnetic and antiferromagnetic orders in Mn-doped CaRuO3
M. Yokoyama, H. Hagiya, N. Oyama, Y. Nishihara, H. Kawanaka
Modulated-structure analysis of the high-valence aperiodic chain compounds,
Sr2k(Co1-xNix)O3 (k˜0.635, 0<=x<=1)
M. Isobe, H. Kitazawa, K. Ohoyama
Magnetic phase diagram under low temperature and high pressure in RVO3
D. Bizen, H. Nakao, K. Iwasa, Y. Murakami, T. Osakabe, S. Miyasaka, Y. Tokura
Study on thermoelectric properties and misfit-structures in Y doped Ca3Co4O9
H.Nakatsugawa, H.M.Jeong, K.Nagasawa
Magnetic excitation in a non-centrosymmetric pressure-induced superconductor
CeRhSi3
N. Aso, H. Miyano, H. Yoshizawa, N. Kimura, T. Komatsubara, H. Aoki
Neutron diffraction under pressure in CeRhIn5
N. Aso, K. Ishii, H. Yoshizawa, T. Fujiwara, Y. Uwatoko, G. F. Chen, N. K. SatoTwo-dimensional magnetic excitations in CeRhIn5
N. Aso, H. Miyano, H. Yoshizawa, G. F. Chen, N. K. Sato
Search for magnetic excitation in a heavy fermion superconductor CeCoIn5
N. Aso, H. Miyano, H. Yoshizawa, T. Fujiwara, G. F. Chen, N. K. Sato
Correlation between ferromagnetism and superconductivity in UGe2
N. Aso, S. Ban, K. Deguchi, T. Fujiwara, Y. Uwatoko, N. K. Sato
Observation of magnetic form factor using detwinned single crystal of La2CuO4
H. Kimura, T. Adachi, Y. Noda, M. Fujita, K. Yamada
Relation between low-energy phonons and a charge stripe order inLa2㺍㺍x Srx Cu1㺍y Fey O4
H. Kimura, Y. Ishikawa, Y. Noda, K. Enoki, M. Fujita, K. Yamada
Search for magnetic scattering in Fe and Pb co-doped Bi2201
H. Hiraka, K. Yamada
Magnetic Correlation in the Kondo-Semiconductor-like Material CeOs4Sb12
K. Iwasa, S. Itobe, M. Kohgi, C. Yang, K. Kuwahara, H. Sugawara, H. Sato, N. Aso
Visualization of rattling in filled skutterudite compounds
K. Kaneko, N. Metoki, H. Kimura, Y. Noda, T. D. Matsuda, M. Kohgi
Magnetic Excitation of Ferromagnetic System NdFe4P12 Exhibiting Heavy
Electron Behavior
K. Iwasa, L. Hao, K. Saito, H. Sugawara, H. Sato
Crystal-field excitation in Pr(Ru1㺍㺍x Rhx )4P12
K. Iwasa, K. Saito, L. Hao, Y. Murakami
Spin-lattice dynamics in rare earth antiferroquadrupolar ordering conpound
HoB2C2
K. Ohoyama , H. Onodera, E. Matsuoka㪄㩷 㪈㪈㩷㪄

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㪈㪄㪊㪄㪉㪈 Coexistence of superconductivity and magnetism in a multi-layered cuprate
C. H. Lee, A. Iyo, K. Kihou, H. Kito, K. Yamada㪈㪄㪊㪄㪉㪉 Flux line lattice in ErNi2B2C
H. K. Furukawa, R. Nagatomo, S. Konno, S. O. Kawamura, H. Yoshizawa, H. Takeya
㪈㪄㪊㪄㪉㪊 Magnetic and electronic nature of metallic ferromagnet Sn2Co3S2 and its related
compounds
M. Matoba, A. Umetani, E. Nagoshi, S. Nakajima, T. Kubodera㪈㪄㪊㪄㪉㪋 Charge and spin ordering in La1.85Ca0.15CoO4.17
K. Horigane, H. Haruhiro, K. Yamada, J. Akimitsu㪈㪄㪊㪄㪉㪌 Lattice effects on the charge-spin ordering in layered cobaltates R1.5Sr0.5CoO4
K. Horigane, H. Haruhiro, K. Yamada, J. Akimitsu㪈㪄㪊㪄㪉㪍 Cycloidal Spin Order in (Gd,Tb)MnO3 with Electric Polarization along the a-Axis
H. Sagayama, N. Abe, K. Taniguchi, T. Arima, Y. Noda, M. Soda, M. Matsuura
K. Hirota, Y. Yamasaki, D. Okuyama, Y. Tokura㪈㪄㪊㪄㪉㪎 Correlation between Electric Polarization and Sence of Helix in MnWO4
H. Sagayama, N. Abe, K. Taniguchi, T. Arima, M. Soda, M. Matsuura, K. Hirota
㪈㪄㪊㪄㪉㪏 Magnetic excitations of NaxCoO2.yD2O
T. Moyoshi, Y. Yasui, M. Sato, K. Kakurai㪈㪄㪊㪄㪉㪐 Magnetic structure of a pressure-induced magnetically ordered phase in YbAgGe
with a quasi-kagome lattice
K. Umeo, H. Kubo, T. Onimaru, K. Katoh, T. Matsumura, N. Aso, T. Takabatake㪈㪄㪊㪄㪊㪇 Spin excitations in MgCr2O4
K. Tomiyasu, H. Suzuki, M. Toki, S. Itoh, N. Aso, M. Matsuura, K. Yamada㪈㪄㪊㪄㪊㪈 Magnetism and superconductivity in RE Ni2B2C
S. O. Kawamura, R. Nagatomo, S. Konno, H. K. Furukawa, H. Yoshizawa
㪈㪄㪊㪄㪊㪉 Electronic state in novel superconductor CeCoIn5 studied by observation of thevortex state
H. K. Furukawa, S. O.Kawamura, S. Konno, R. Nagatomo, H. Shishido, T. Shibauchi
Y. Matsuda㪈㪄㪊㪄㪊㪊 Investigation of the magnetic excitations in high-TC
M. Matsuura, Y. Yoshida, H. Eisaki, N. Kaneko, K. Hirota
㪈㪄㪊㪄㪊㪋 Magnetic Structure in the Shastry-Sutherland Lattice Tb1-xYxB4
F. Iga, S. Michimura, K. Murakami, T. Takabatake, K. Suga, K. Kindo, K.Ohoyama㪈㪄㪊㪄㪊㪌 1st order transition in ErNi2B2C
H. K. Furukawa, Y. Ishida , S. O. Kawamura, H. Yoshizawa, H. Takeya
㪈㪄㪊㪄㪊㪍 Study of spin fluctuations in La1.94-x Srx Ce0.06CuO4
M. Fujita, M. Enoki, K. Yamada㪈㪄㪊㪄㪊㪎 Search for transition of paring symmetry in electron-doped superconductor
Pr1㺍㺍x LaCex CeO4
M. Fujita, M. Nakagawa, K. Yamada㪈㪄㪊㪄㪊㪏 Zn-doping effect on spin fluctuations in electron-doped Pr1㺍㺍x LaCex CuO4
M. Fujita, M. Nakagawa, K. Yamada㪈㪄㪊㪄㪊㪐 Order Parameter of Phase IV in (Ce,La)B6
K. Kuwahara, K. Iwasa, M. Kohgi, N. Aso, M. Sera, F. Iga, M. Matsuura, K. Hirota
㪈㪄㪊㪄㪋㪇 Neutron scattering study on PrFe4P12 under high pressure
K. Kuwahara, T. Osakabe, K. Iwasa, M. Kohgi, D. Kikuchi, Y. Aoki, H. Sato, H.Sugawara
㪈㪄㪊㪄㪋㪈 Rattling motion in PrOs4Sb12
K. Kuwahara, O. Yamamuro, K. Iwasa, M. Kohgi, D. Kikuchi, Y. Aoki, H. Sato, H.Sugawara㪄㩷 㪈㪉㩷㪄

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Neutron Scattering -Amorphous 䊶 LiquidDirect observation of supercooled water in hardened Low Heat Portland Cement
K. Mori, Y. Inamura, O. Yamamuro, T. Fukunaga
Neutron Diffraction Study on the Intermolecular Structure in Highly Concentrated
Aqueous Urea Solutions
Y. Kameda, A. Maki, H. Takahashi, Y. Amo, T. Usuki
SANS Study on Mixing State of Ionic Liquid-Molecular Liquid Binary Solutions
T. Takamuku, Y. Honda, K. Fujii
Amide-Induced Phase Separation of HFIP-Water Mixtures
T. Takamuku, H. Wada, K. Fujii
Alkyl-chain Dependence on Micro-phase Separation of Room Temperature Ionic
Liquids
K. Fujii, Y. Umebayashi, S. Ishiguro, T.Takamuku
Structural Change of Supercritical Carbon Dioxide with Entrainer Molecule
T. Sato, M. Sugiyama, M. Misawa, K. Hamada, K. Itoh, K. Mori, T.Fukunaga
Static and Dynamic Structure of Meso-scale fluctuations in liquid chalcogens near
the metal-nonmetal transition
Y.Ohmasa, T.Hoshino R.Osada, M.Yao
Small Angle Neutron Scattering Investigation of Aggregation ofN,N-dialkylamide and Its Effect on Nitric Acid Extraction
S. Suzuki, T. Yaita, R. Motokawa, S. Koizumi㪄㩷 㪈㪊㩷㪄

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䇸䇭T i t l e䇭䇹
Neutron Scattering - Polymer Dynamical Study on Nanocomposite Hydrogel by Means of Neutron Spin Echo Technique
H. Endo, S. Miyazaki, M. Shibayama
Hysteresis of bicelle/ULV transition in long- and short-chain lipid mixture
N. L. Yamada, N. Torikai
Changes in flow-induced aggregated structures of shear-thickenning silica suspensions
M. Ando, H. Mizukawa, Y. Takahashi, M. Kawaguchi
Simultaneous Evaluation of Lipid Exchange and Flip-Flop in Vesicles
Nakano, M. Fukuda, T. Kudo, H. Endo
Structure Analyses of Nanoemulsion/polymer Mixtures Having Dilatancy Behavior
M. Shibayama, Y. Kawada, T. Kume, H. Endo, N. Osaka. N, T. Matsunaga
Ionic Strength Dependence of Chain Conformation of Hydrophilic Polymers at
Water Interface
M. Kobayashi, Y. Terayama, N. Hosaka, A. Takahara
Surface and Interface Structure Analysis of (Multi-functionalized
Silsesquioxane/Deuterated Polystyrene) Hybrid Thin Films
N. Hosaka, Y. Terayama, M. Kobayashi, A. Takahara
Thermal fluctuation of a lipid bilayer in the anomalous swelling regime
M. Hishida, H.䇭Seto, N. L. Yamada
Melting and Re-crystallization Process of Shish-kebab Structure
G. Matsuba, Y. Hayashi, C. Ito, K. Nishida, T. Kanaya
Gelation Mechanism of Clay-Polymer Nanocomposite Hydrogel using Contrast
Variation SANS
M. Shibayama, S. Miyazaki , H. Endo , T. Karino , K. Haraguchi
Structural Formation Process under Drawing
K. Nishida, T. Kanaya, G. Matsuba, Y. Hayashi, C. Ito
Distribution of glass transition temperature in polymer thin films by neutronreflectivity
R. Inoue , H. Ogawa, T. Kanaya, K. Nishida , M. Hino
A long-range periodic structure in a mixture of D2O/3-methylpyridine/NaBPh4
induced by solvation effect
K. Sadakane, N. Iguchi. H. Seto
Effect of polymer on uni-lamellar vesicle in lipid mixture system
N. L. Yamada, N. Torikai
Studies on Structural Nonuniformity of Natural Rubber
M. Shibayama , T. Suzuki, N. Oosaka, H. Endo, N. Higashitani, Y. Morita, Y. Kokubo
Y. Ikeda, S. Kohjiya
Temperature Effects on Shear-Induced Structural Transition in the Lamellar Phaseof a Nonionic Surfactant -Change in the Orientation of LamellaeY. Kosaka, M. Ito, Y. Kawabata, T. Kato
Correlation between local dynamics and gas permeability of substitutedpolyacetylenes by quasielastic neutron scattering
T. Masuda, T. Kanaya, R. Inoue, O. Yamamuro
Crowding effect on the shear induced structural transition of lamellar phase
S. Fujii, Y. Kawabata
Nanostructure of Non-Surface Acitive Ionic Amphiphilic Diblock Copolymers in
Aqueous Solutions
H. Matsuoka, H. Chen, F. Ozaki, T. Yamada
2D-SANS Pattern Observed for Injection Molded Isotactic Polypropylene
T. Sakurai, Y. Nozue, S. Kimata, T. Kasahara, N.Yamaguchi, H. Endo, M. Shibayama㪄㩷 㪈㪋㩷㪄

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㪈㪄㪌㪄㪉㪈 Dynamical Properties of Syndiotactic Polystyrene (sPS) Crystalline Complex Phase
F. Kaneko, T. Kawaguchi, K. Ute
㪈㪄㪌㪄㪉㪉 Electrostatic Self-Assembly of Neutral and Polyelectrolyte Block Copolymer andOppositely Charged Surfactant
M. Annaka, T. Matsuda, K. Morishita㪈㪄㪌㪄㪉㪊 Effects of Molecular Weight and Surface Density on Conformation ofPoly(N-isopropylacrylamide) Brushes Immobilized Onto A Substrate
M. Annaka, Y. Fujii, H. Atarashi, K. Tanaka, T. Nagamura, M. Hino㪈㪄㪌㪄㪉㪋 Analysis of Adsorption Behavior for Proteins onto (Liquid/Polymer) Interface
Y. Fujii, H. Atarashi, K. Tanaka, T. Nagamura, M. Hino㪈㪄㪌㪄㪉㪌 Lamellar to Micelle Transition of Nonionic Surfactant Assemblies Induced byAddition of Colloidal Particles
Y. Suganuma, N. Urakami, R. Mawatari, S. Komura, K. N. Yaegashi, M. Imai㪈㪄㪌㪄㪉㪍 Nano-meter-sized domain formation in lipid membranes observed by small angle
neutron scattering
Y. Sakuma, M. Imai, T. Masui, N. Urakami㪈㪄㪌㪄㪉㪎 Sol-Gel Transition of Hydrophobically Modified Polyrotaxane
T. Karino, Y. Okumura, C. Zhao, M. Kidowaki, T. Kataoka, K. Ito, M. Shibayama㪈㪄㪌㪄㪉㪏 Structural Study on Uniaxial Extension of Nanocomposite Hydrogel with HighClay Concentration by Means of Contrast Variation Neutron Scattering
T.Nishida, H. Endo, N. Osaka, K. Haraguchi, M. Shibayama㪄㩷 㪈㪌㩷㪄

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䇸䇭T i t l e䇭䇹
Neutron Scattering - Biology Control of Membrane Lipid dynamics by Transmembrane and Amphipathic Peptides
M. Nakano, M. Fukuda, T. Kudo, H. Endo
Dynamics of folded and partial unfolded proteins observed by solution inelastic
neutron scattering
H. Nakagawa, Y. Joti, O. Yamamuro, I. Tsukushi, M. Kataoka
Hydration water dynamics at protein dynamical transition by quasi-elastic neutron
scattering
H.Nakagawa, Y.Joti, O.Yamamuro, M.Kataoka
Strctural torlance of complex of A-crystallin and B-crystallin
M. Sugiyama, N. Fuji, Y. Morimoto, T. Sato
Measurements of slow dynamics of actin
S. Fujiwara, F. Matsumoto, H. Nakagawa, N. Takahashi, T. Oda
Structure and dynamics of -lactoglobulin aggregates by small-angle neutron
scattering and neutron spin echo methods
K. Yoshida, T. Yamaguchi, H. Endo, M. Shibayama
Neutron Diffraction Study of HIV-1 Protease in Complex with Inhibitor KNI-272
M. Adachi, T. Ohhara, K. Kurihara, T. Tamada, E. Honjo, N. Okazaki, S. Arai, Y. Shoyama
H. Matsumura, H. Adachi, K. Takano, Y. Mori, K. Hidaka, T. Kimura, Y. Hayashi, Y. Kiso
R. Kuroki
Neutron Diffraction Study of ADP-ribose pyrophosphatase
M. Adachi, K. Kurihara, T. Tamada, T. Ooga, S. Kuramitsu, R. Kuroki
Trial Diffraction Measurements of Protein Single Crystals in H 2O
S. Fujiwara, K. Kurihara, T. Chatake
The State of Cryptobiosis of Larvae of Polypedilum Vandezplanki Studied by
Incoherent Inelastic Neutron Scattering
H. Nakagawa, T. Okuda, M. Kataoka
Dynamical Transition of DNA Studied by Neutron Inelastic Scattering
H. Nakagawa, H. Kono
Glass Transition of Larvae of Polypedilum Vandezplanki Studied by Incoherent
Inelastic Neutron Scattering
H. Nakagawa, T. Okuda, M. Kataoka
Contrast Variation Measurements of Hen Egg White Lysozyme Amyloid Fibrils
S. Fujiwara, F. Matsumoto, H. Nakagawa
Small-Angle Neutron Scattering Measurements of Rhodanase-GroEL-GroES
ComplexK. Ichimura, Y. Matsuura, S. Fujiwara, Y. Kawata, H. Kihara
Small-Angle Neutron Scattering Measurements of  -Synuclein and its
Disease-Related Mutants
S. Naito, H. Mochizuki, T. Yasuda, J. Yamaguchi, Y. Mizuno, M. Furusaka, S. Ikeda
M. H. Shimizu, S. Fujiwara㪄㩷 㪈㪍㩷㪄

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Neutron Scattering - Fundamental Physics䊶 Neutron Optics Development of phase correction devices for high resolution NRSE spectrometer
M. Kitaguchi, M. Hino, Y. Kawabata, H. Hayashida, S. Tasaki
Development of Jamin Type Cold Neutron Interferometer with Completely Separated
Two Paths
Y. Seki, K. Taketani, H. Funahashi, M. Kitaguchi, M. Hino, Y. Otake, H.M. Shimizu
Development of beam splitting etalons for pulsed neutrons II
M. Kitaguchi, Y. Seki, K. Taketani, H. Funahashi, M. Hino, H. M. Shimizu
Possible improvement of thin magnetic film using Pd
S. Tasaki, S. Kuramoto, Y. Abe, M. Hino
Development of neutron optics with a curved supermirror
K. Ikeda, H. Sato, K. Hirota, K. Mishima
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Neutron Scattering - Instrument 㪈㪄㪏㪄㪈 Thermal diffuse scattering effect on neutron holography
K. Hayashi, K. Ohyama, S. Orimo, Y. Nakamori, H. Takahashi, K. Shibata㪈㪄㪏㪄㪉 Development of A New Spin-Phase Contrast Imaging of Neutron
S. Tasaki, M. Kageyama, M. Hino, Y. Kawabata㪈㪄㪏㪄㪊 Development of transmittion geometry supermirror polarizer
M.Hino, M.Kitaguchi, H.Hayashida, Y.Kawabata, S. Tasaki㪈㪄㪏㪄㪋 Observation of superparamagnetic fluctuations in magnetic ferrofluid using
MIEZE spectroscopy
M.Hino, H.Hayashida, M.Kitaguchi, N.Achiwa, Y. Kawabata㪈㪄㪏㪄㪌 Installation of a prototype of focusing-type small-angle neutron scattering
instrument with an ellipsoidal supermirror
M. Furusaka, T. Satoh, Y. Sasaki, Y. Kawamura, T. Asami, Y. Otake, K. Ikeda
P. Mikula, Y. Kiyanagi, S. Naito, H. Yoshizawa
㪈㪄㪏㪄㪍 Development of 10 GPa class cubic anvil type high pressure apparatus for neutron
scattering experiments
T. Fujiwara, K. Matsubayashi, Y. Uwatoko, N. Aso, M. Nishi, H. Yoshizawa
㪈㪄㪏㪄㪎 Development of Large 2D-PSD under collaboration with HANARO
Y. Noda, M.Watanabe, H. Kimura, Y. Dohi, Y. Ishikawa, T. Yamazaki, M. Moon
C. H. Lee㪈㪄㪏㪄㪏 Neutron imaging measurement using newly developed inorganic gadolinium
scintillator
J. H. Kaneko, S. Satoh, J. Haruna, S. Saeki, S. Kawamura, Y. Ohtake, M. Furusaka
Y. Kiyanagi㪈㪄㪏㪄㪐 Performance Test of Neutron Detector for Engineering Diffractometer in J-PARC
K. Sakasai, T. Nakamura, S. Harjo, A. Moriai, M. Katagiri, K. Soyama, S. SatohE. Shooneveld, N. Rhodes3㪈㪄㪏㪄㪈㪇 Development of He PSDs and Related Electronics for New Spectrometers in J-PARC
K. Nakajima, T. Yokoo, S. Satoh, K. Shibata, N. Takahashi, R. Kajimoto, T. Nakatani
Y. Inamura, N. Kaneko, Y. Yasu, K. Nakayoshi, E. Inoue, H. Sendai, M. Arai㪈㪄㪏㪄㪈㪈 Development of Asymmetric Reflection-type Germanium Monochromatorfor Beam Flux Enhancement on HRPD
H. Yamauchi, Y. Ishii, N. Igawa, H. Fukazawa, W. Utsumi
㪈㪄㪏㪄㪈㪉 Development of High Quality Neutron Mirrors with Upgrading Compact Cold
Neutron Bender System II
I. Tamura, R. Maruyama, D. Yamazaki, K. Yamamoto, K. Nakamura, K. Soyama㪈㪄㪏㪄㪈㪊 Development of High Reflectivity Neutron Supermirror Using Ion Beam Sputtering
TechniqueR. Maruyama, D. Yamazaki, T. Ebisawa, K. Soyama㪈㪄㪏㪄㪈㪋 Neutron Reflectometer SUIREN: Status and Developments in 2007
D. Yamazaki, M. Takeda, R. Maruyama, M. Hino, K. Soyama㪈㪄㪏㪄㪈㪌 Upgrading Compact Cold Neutron Bender System II
I. Tamura, R. Maruyama, D. Yamazaki, K. Yamamoto, K. Nakamura, K. Aizawa, K. Soyama㪈㪄㪏㪄㪈㪍 Neutron Detection by a MgB2 Transition Edge sensor
S. Okayasu, M. Katagiri, K. Houjo, Y. Morii, S. Miki, H. Shimakage, Z. Wang, T. Ishida㪈㪄㪏㪄㪈㪎 Application of a Magnetic Neutron Polarizing and Focusing Device to a
Focusing-Geometry Small-Angle Polarized Neutron Scattering Instrument
T. Oku, T. Shinohara, T. Kikuchi, Y. Oba, H. Iwase, S. Koizumi, J. Suzuki㪄㩷 㪈㪎㩷㪄

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Neutron Scattering - Superconductivity Emergence of Magnetic Modulations in the Overdoped Phase of Bi2201 by
by Fe Doping
H. Hiraka, S. Wakimoto, M. Takeda, K. Kakurai, K. Yamada
Peculiar Field Response of Antiferromagnetism in non-centrosymmetricheavy fermion superconductor CePt3Si
K. Kaneko, N. Metoki, T. Takeuchi, T.D. Matsuda, Y. Haga, R. Settai, Y. Onuki
䇸䇭T i t l e䇭䇹

Neutron Scattering - Residual Stress 㪈㪄㪈㪇㪄㪈 Strain Evaluation of Rebar in Reinforced Concrete Using Neutron Diffraction
M. Kanematsu, T. Noguchi, M. Yasuda, H. Suzuki㪈㪄㪈㪇㪄㪉 Residual Stress and Deformation Behavior on Zr55Al10Ni5Cu30
Bulk Metallic Glass Containing ZrC Particles
H. Suzuki, J. Saida, M. Imafuku㪈㪄㪈㪇㪄㪊 Bulky Measurement of Gradient Texture of an IF Steel by Neutron Diffraction
P.G. Xu, Y. Tomota, H. Suzuki, S. Machiya㪈㪄㪈㪇㪄㪋 Engineering diffractometer ”RESA” and ”RESA-II”
H. Suzuki, T. Saito, S. Machiya, Y. Tsuchiya, A. Moriai, Y. Shimojo, K. Akita, Y. Morii㪄㩷 㪈㪏㩷㪄

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䇸䇭T i t l e䇭䇹
Neutron Radiography
Fundamental Experiments for the Development of an Advanced Neutron
Tomography
M. Kureta
Development of an Ultra-High-Speed Scanning Neutron Tomography
System for High-Quality and Four-Dimensional Visualizations
M. Kureta, H. Iikura
Development of Measurements for Multiphase Flow Dynamics -II by Using
Neutron Beam of JRR-3M
K. Mishima
Defense Responses of Trees and Dynamics of Water Distribution
T. Yamada, N. Nagaishi, K. Tanoi, T.M. Nakanishi
Development of Imaging System for Neutron Image Intensifier
K. Mochiki, Y. Wada, M. Okazaki
Analysis of water distribution in plant tissue.
T. Nakanishi

䇸䇭T i t l e䇭䇹Prompt Gamma-ray Analyses
Development of a Method of Measuring the Cadmium Concentrationin Agricultural Produce with Prompt γ-ray Analysis
Y. Sakurai, H. Matsue, S. Miyamoto, N. Kihou
Measurements of Hydrogen-Containing Samples Using MPGA
Y. Toh, M. Oshima, M. Koizumi, K. Furutaka, A. Kimura, Y. Murakami
Determination of Boron in Ceramic Reference Materials by Prompt
Gamma-ray Analysis Using Focused Neutron Guided Beam of JRR-3M
T. Miura, H. Matsue, T. Kuroiwa, K. Chiba
Non-Destructive Analysis of Ancient Egyptian Vitreous Relics by Neutron
S. Yoshida..
Development of Temperature Variable Neutron In-beam Mossbauer
Spectrometer
M. K. Kubo, Y. Kobayashi, Y. Yamada, Y. Watanabe, T. Takayama, Y. Sakai
H. Shoji, W. Sato, A. Shinohara, M. Segawa, H. Matsue㪄㩷 㪈㪐㩷㪄

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Neutron Activation Analyses
129
Survey of I concentration in soil around the Tokai Reprocessing Plant
Y. kokubun, M. nakano, M. Takeishi
Influence of water concentrations to chemical forms of tritium generated in mercury through anuclear reaction
K. Manabe, S. Yokoyama
Analysis of element in annually layered terrestrial carbonates (Tufa )S. Sugihara, I. Morinaga, A. Hirose
Studies on Phytoremediation of Soil Pollutions at the trace of a factory
Y. Kawanishi, N. Nogawa, Y. Makide, H. Sawahata, M. Kawate, M. Ishimoto, H. Matsue
Instrumental Neutron Activation Analyses of volcanic rocks from Kyushu island:
Characterization of Material Circulation through Volcanism
T. Hasenaka, M. Miyoshi, T. Nasu, M. Shimono, T. Edamura, K. Tanida, Y. Sekiguchi
M. Morinaga, Y. Takae, H. Uemura
Origin and fate of arsenic in volcanic hot spring area
Y. Kikawada, T. Oi, T. Hyatsu, J. Sano, A. Inoue, K. Oda, H. Fuji, Y. Ohno, K. Kyomen, N. Sato
Accumulation of elements in an arable field with soil amendments (organic un-usedresources) and its uptake by cultivated crop
H. Suzuki, H. Kumagaya, N. Nogawa

䇸䇭T i t l e䇭䇹OthersBoron neutron capture therapy for head and neck malignancies.
J. Hiratsuka, T. Aihara, M. Uno, H. Kumada, K. Ono, T. Harada
Study of Hyperfine Interaction using βray detected NMR-ON
S. Ohya,T. Ohtsubo, T. Izumikawa, S. Muto, K. Nisimura
Basic & Clinical Research for Application of Neutron Capture Therapy
to Highly Advanced Cancer
H. Yanagie, S. Mikado, N. Yasuda, S. Higashi, I. Ikushima, R. Mizumachi, Y. Murata, Y. Morishita
A. Shinohara, K. Ogura, H. Sugiyama, N. Ryohei, S. Takamoto, M. Eriguchi, H. Takahashi
Basic & Clinical Research for Application of Neutron Capture Therapy
to Highly Advanced Cancer
H. Yanagie, K. Kakimi, A. Hosoi, A. Ogata, K. Mouri, K. Eguchi, Y. Morishita, A. Shinohara,
H. Kumada, T. Nakamura, Y. Furuya, S. Takamoto, M. Eriguchi, H. Takahashi㪄㩷 㪉㪇㩷㪄

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1.  ਛᕈሶᢔੂ 1 ᭴ㅧ࡮ബ⏛ 


1. Neutron Scattering

1 Structure࡮Excitation㻙㻌 㻞㻝㻌㻙This is a blank page.

JAEA-Review 2011-050

1-1-1
Correlation between structural and thermoelectric properties in Zn13Sb10
G. Nakamoto(A), A. Tada(A), M. Kurisu(A), A. Tanaka(B), T. Tsutaoaka(B), Y. Andoh(C)(A)Japan Advanced Institute of Science and Technology, Ishikawa 923-1292, Japan,(B)Graduate School of Education, Hiroshima University, Hiroshima 739-8524, Japan,(C)Faculty of Regional Sciences, Tottori University, Tottori 690-8550, Japanried out at T1-3 HERMES in JRR-3M atroom temperature with a wave length of
1.82646(6) A. The data were collected by an
MFC mode.
Figure 1 shows the powder neutron
diffraction proﬁle and result of Rietvelt
analysis of the Zn13Sb10 GF ingot at room
temperature. The Rietveld analysis was
performed by using a pattern proﬁle ﬁttig program RIETAN-2000. Any reﬂections
from an impurity phase are not detected.
All the reﬂection peaks can be indexed byassuming a rhombohedric hexagonal structure (R3-c). The lattice parameters determined by this analysis are in good agreement with that obtained by the previous Xray diffraction experiment. The goodnessof ﬁt, S, is obtained to be 1.40 at present.
However, the relative intensity of the reﬂection peaks is not well ﬁtted. This may
be due to the difference in occupation of
Zn atom at the interstitial sites from thestarting structure model proposed by othergroups. More presice analysis is now under
way to determine the site occupancy especially for Zn atoms and to discuss the correlation between structural and thermoelectric properties of Zn13Sb10 compound.
3000

Zn13Sb10 at R.T.
2000

Intensity (cps)beta-Zn13Sb10 compound has been wellknown as a good thermoelectric material
in the moderate temperature range becauseof its high dimensionless ﬁgure of merit,
ZT=1.3 at 670 K. The high thermoelectric performance of this material originates
mainly from the extremely low-thermal
conductivity. Recently, it has been reported
that such an extremely low-thermal conductivity is attributed to the disorderedstructure of Zn atoms or rattling motion of
Sb-dimmers along the c-axis. However, theorigin of the extremely low-thermal conductivity still remains an unresolved problem. More recentrly, it has been revealed
that the occupation of Zn atoms at the interstitial sites has also strong inﬂuence on the
structural property as well as thermoelectric one. Especially, the alpha to beta structural transtion at 260 K is largely dependent on Zn composition. Thus, there aremany problems left about the correlation
between the structural and thermoelectric
properties of Zn13Sb10 compound.
In this experiment, powder neutron
diffraction measurements were performed
to examine the detailed crystal structure of
Zn13Sb10 compound to clarify the correlation between the structural and thermoelectric properties.
Polycrystalline ingots were prepared bygradient freeze (GF) and vacuum-melt toquench (VMQ) methods. The constituent
elements of Zn(5N) and Sb(6N) with thestoichiometric ratio 13:10 were encapsulated in a double quartz ampoule undervacuum. The GF ingot was grown in a vertical GF furnace at the growth rate of 3
mm/day. On the other hand, the VMQ ingot was melted in an electric furnace for
2 days and then quenched into ice water.
Neutron diffraction experiment was car-

1000

0

20

40

60

80
2θ (deg.)

100

120

140

Fig. 1. Powder neutron diffraction proﬁle and resultof Rietveld analysis for Zn13Sb10 at room temperature.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 285

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Dynamics of the water included in [H11O5][ZnCu(CN)4]
Sin-ichi Nishikiori(A), Yoko Minamimoto(B), Osamu Yamamuro(B)(A) Dept. of Basic Science, Graduate School of Arts and Sciences, Univ. Tokyo, (B) ISSP-NSL
Univ. Tokyo
The
title
compound[H(H2O)5][ZnCu(CN)4] is a bimetal
cyanide complex with a 3D framework
structure built by bidentate behavior of
cyanide linking tetrahedral Cu(I) andZu(II) ions. The structure of the 3D framework is the tridymite-like structure asshown in Fig. 1 and the framework has
negative electric charges. Inside the 3D
framework void space is formed and watermolecules and protons are included. The
water molecules and protons are considered to form a hydrogen bonding network
which penetrates the 3D framework of thebimetal cyanide complex. Although ourprevious X-ray structure analysis revealed
the 3D framework structure, the structureof the hydrogen bonding network was
unclear. The water molecules and protons
are expected to be in a dynamic state.
DSC measurement showed phase transitions at 160K-170K and 240K. 2H-NMR
powder patters, which were measured
using a deuterated sample, suggested aﬂip-ﬂop motion about the C2 axis of awater molecule below 168K, a rotationalmotion about the C2 axis between 178K
and 233K and an isotropic rotational motion above 253K for the water molecules.
Although considerably activated rotationalmotion was conﬁrmed near room temperature, there was no information abouttranslational diffusion of the protons. If
translational diffusion is observed, a possibility as a proton conductor comes up.
In order to obtain information about suchtranslational diffusion, we have carried out
quasi-elastic neutron scattering (QENS)
measurement on the title compound.
The sample was powdered and packed
in a double walled cylindrical cell madeof Al. The shape of the packed sample
was a cylinder with a 13 mm diameter,

a 50 mm height and a 1 mm thickness.
The QENS measurement was carried out inthe temperature range of 200K-323K on atime-ﬂight type spectrometer AGNES(C31-1) installed at JRR-3M on JAEA(Tokai).
The data obtained were analyzed using
the Chudley-Elliott model after several trials. This model is a jump diffusion modelin which an atom stays and vibrates at agiven position for an interval time and afterthat time the atom jumps rapidly to anotherposition. In the case of a powder sample
the jump direction is isotropic but the jump
distance is ﬁxed to a constant value. In
our case, considering the results of the 2HNMR experiments, we assumed that during the interval time the proton is undergoing reorientation among the four apexesof a tetrahedron which is a part of the hydrogen bonding network formed with thewater molecules. At the center of the tetrahedron the O atom of a water molecule ispositioned and the distance between the O
and each apex is 0.97 A, which is the bondlength of O-H. Fig.2 shows the HWHM vs
Q plot and the best ﬁt results based on our
Chudley-Elliott model for the translational
diffusion. From this ﬁtting, the jump distance, the interval time, the diffusion constant and the activation energy were derived to be 2.9(1) A, 9(3) x 10ˆ-15 sec, 6(3)x 10ˆ13 Aˆ2/sec and 16(1) kJ/mol, respectively. Considering the O-O distance in a
O-H-O type hydrogen bond is 2.72(15) A,
the jump distance obtained here means thatthe proton diffuses by a jump to an adjacentwater molecule. The correlation time andthe activation energy for the 4-site reorientation during the interval time were calculated to be 1.7(3) x 10ˆ-12 sec and 11.2(5)kJ/mol, respectively.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 327

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1-1-2

Fig. 1. Fig.1. The structure of the 3D framework of[ZnCu(CN)4]-. Fig.2. HWHM vs Q plot and curve
ﬁtting using the Chudley-Elliott model for the translational diffusion.

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JAEA-Review 2011-050

1-1-3Structural phase transition of one-dimensional semiconductor C5 H10 NH2 PbI3
M. Takahashi1 , K. Kawasaki1 , K. Kataoka1 , Y. Fujii1 , M. Watanabe2 ,K. Ohshima1 and Y. Noda2
Inst. of Mat. Sci., Univ. of Tsukuba1 , IMRAM, Tohoku Univ.2
Structural phase transition of onedimensional lead-based inorganic-organic
perovskites C5 H10 NH2 PbI3 has beenstudied by using a single crystal diffractometer T2-2, FONDER. C5 H10 NH2 PbI3
consists of semiconducting part composed of one-dimensional inorganic chainsand barrier parts composed of inorganic
Studies with
C5 H10 NH2+ molecules.
Raman scattering, DSC and optical absorption have shown that the material exhibits
temperature-induced phase transitions
involving rotational/orientational ordering of C5 H10 NH2+ molecules below room
temperature. For detailed information on
the structure of inorganic part, neutron
diffraction measurement is indispensable.
Crystal structure at room temperature isdetermined by combination of X-ray andneutron analysis. Positional parameters for
Pb and I are ﬁxed by x-ray analysis [2]and those of atoms in inorganic parts are
determined by 200 neutron intensity datawith R values of 0.068. Figure 1(a) shows
nuclear density distribution on (001) planewith equicontour surface at ±0.8 f m/Å calculated by MEM. It clearly shows negative peaks (blue part) which indicate hydrogen atom positions. Nuclear density at
6-ring C5 N is found to be higher for thesites closer to the inorganic chains, indicating that N atom tends to occupy the closer
sites to the semiconducting part.
Figure 1(b) shows temperature dependence of lattice parameters. It shows steplike changes at the transition temperatureswith considerble large contraction of latticeb. Below 285K, 400 peak separates in two
indicating that the crystal lattice changes
from orthorhombic to monoclinic symmetries. The temperature dependence of angle α of the monoclinic lattice is shown in
Fig.1(c). The results show that the succes-

sive phase transitions accompanied withlarge structural change take place below
the room temperature. Further study todetermine the structure at each phase is inplanning.
[1] A. Masui et al.: Phys. Stat. Sol. (b) 223(2001)501.
[2] G. V. Gridunova et al. : Soviet Physics,
Doklady Akademii Nauk SSSR 278, 656(1984).

Fig. 1. (a)Nuclear density distribution on (001)plane.(b)Temperature dependence of lattice parameters. (c)Temperature dependence of angle α of themonoclinic lattice.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 352

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Superspace Group Approach to the Crystal Structure of Chimney-LadderCompound [Mn][Si]gYuzuru Miyazaki, Dai Igarashi and Tsuyoshi Kajitani
Department of Applied Physics, Graduate School of Engineering, Tohoku University
Higher manganese silicide HMS (MnSi2x) exhibits relatively high thermoelectric(TE) performance with the dimension-lessﬁgure-of-merit ZT = S2T/rho/kappa ˜0.7
around 800 K, where S, rho, kappa andT are the Seebeck coefﬁcient, electrical resistivity, thermal conductivity and absolutetemperature, respectively. Due to the natural abundance of constituent elements andhigh-temperature oxidation resistance, thecompound is regarded as a potential p-type
TE material. However, detailed structureof the compound has not been revealed dueto the incommensurate superstructure. In
this study, the crystal structure of HMS
has been determined by means of the (3+1)dimensional superspace group approach.
Neutron powder diffraction (ND) measurement was carried out by means of HERMES diffractometer. Structural parameters
have been reﬁned with a superspace groupof I41/amd(00gamma)00ss using the Rietveld reﬁnement program JANA2000 designed for modulated structure analyses.

pound, t’ is deﬁned as -gx3 + x4˜ -1.74x3+ x4. The coordinates x3 and x4 respectively correspond to the z coordinate in
the [Mn] and [Si] subsystems. The modulation in Mn-Mn distances is relatively
small, ranging from 2.913(9) angstrom to
3.062(15) angstrom. Reﬂecting the large
in-plane modulation of Si atoms, the MnSi distances are signiﬁcantly modulated,from 2.255(12) angstrom to more than 5
angstrom. Such a large modulation would
be an origin of the observed low lattice
thermal conductivity.

The compound can be regarded as a composite crystal which consists of tetragonal[Mn] and [Si] subsystems, with an irrational c-axis ratio (misﬁt parameter) g =c Mn/c Si˜ 1.74. The structure formula canbe expressed as [Mn][Si]g. On the basis of
the adopted superspace group, the modulated structure has been satisfactorily determined, by considering up to 4th ordermodulation amplitudes. A signiﬁcant inplane rotational modulation has been revealed in the ”chimney”-[Si] subsystem,
while the positional modulation in the”ladder”-[Mn] subsystem is less marked.
Fig.1 shows the Mn-Mn and Mn-Si interatomic distances plotted against an internal coordinate t’. In the present comActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 370

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JAEA-Review 2011-050

1-1-5Structure analysis of trehalose dihydrate by neutron diﬀraction
M. Takahashi1 , K. Kawasaki1 , K. Kataoka1 , M. Watanabe2 ,K. Ohshima1 and Y. Noda2
Inst. of Mat. Sci., Univ. of Tsukuba1 , IMRAM, Tohoku Univ.2
α, α-trehalose dihydrate is a nonreducing disaccharide, and very attractivefrom both academic and practical pointsof view, such as an additive for long term
storage in food and pharmaceutical industries. It has high superiority as a protectorof biological molecules compared withother carbohydrates such as sucrose. To
understand the biological protective mechanism of α, α-trehalose, information on thehydrogen atom positions is indispensable.
Structure analysis of α, α-trehalose atroom temperature was carried out bymeans of neutron diffraction method. Intensity data up to sin θ/λ < 0.75Å was collected using crystals with approximate dimensions of 15 × 4.5 × 2.7mm3 by a fourcircle diffractometer, FONDER at T2-2. The
space group of α, α-trehalose is orthorhombic P21 21 21 ( Z = 4) and the obtained lattice
parameters at 300 K were a = 12.2380Å,b = 17.9087Å and c = 7.6032Å. Leastsquare ﬁtting analysis were performed toreﬁne structural parameters; in the analysis, parameters obtained by previous Xray study[1,2] were used as initial parameters for atoms except for the hydrogenatom. Structure determined by 1711 neutron intensity data with R values of 0.068
is shown in Fig.1. Position of hydrogenatoms in both glucose(pink circle) and water molecules(red circle) are determined forthe ﬁrst time. It is found that the hydrogen atoms in water molecules are oriented to the glucose molecules, indicatingthat the molecules are connected to eachother through the hydrogen bonding between the molecule and hydrogen atoms inwater.
[1] G. M. Brown et al. Acta Crystallogr., B
283(1972)3145.
[2] G. Taga et al. Acta Crystallogr., B
283(1972)3258.

Fig. 1. Crystal structure of α, α-trehalose determinedby neutron analysis. Hydrogen atom in glucose andwater molecules are shown with pink and blue circles, respectively.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 373

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JAEA-Review 2011-050

1-1-6

QENS studies of Fast Molecular Reorientation in Liquid, Glass and Crystalline
Phases of 8*OCB
H. Suzuki(A), A. Inaba(A), J. Krawczyk(B), M. Massalska-Arodz(B), T. Kikuchi(C), O.
Yamamuro(C)(A)Osaka Univ., (B)Inst. Nuclear Physics, Krakow, Poland, (C)ISSP-NSL, Univ. Tokyo
Chain branching and chirality ofmolecules affect various physical properties substantially, such as phase behavior.
Some of cyanobiphenyl compounds aregood examples whose phase behavior
varies depending on the presence ofbranch (chirality) in the alkyl side chain.
We have been interested in their phaserelation and dynamics. Here, we report
the results obtained from quasielastic
neutron scattering (QENS) measurements for (S)-4-(1-methylheptyloxy)-4cyanobiphenyl (8*OCB) which is one ofsuch cyanobiphenyl compounds.
Various kinds of measurements have already been made for 8*OCB. From thecalorimetric measurements [1] and IR spectroscopy [2], the phase behavior of 8*OCB
was established. The isotropic liquid is easily undercooled and forms glassy state on
further cooling below 218 K. There exist
two crystalline phase (metastable and stable). This phase behavior is entirely different from that of the non-chiral isomer,
8OCB, which has two liquid crystal phases(nematic and smectic). The dielectric relaxation measurements [3] have also been
made, and they showed that the molecularreorientation around its short axis becomesquite slow near the glass transition temperature at 218 K. The purpose of this experiment was to investigate the molecular reorientation around its long axis and the internal molecular motions.
We performed QENS experiments on
8*OCB using AGNES spectrometer at JRR3M. The measurements were made at 370
K, 350 K, 330 K, 310K, 290 K, 270 K
for isotropic liquid phase with a lowresolution mode (delta E = 120?micro-eV).
As a reference sample, 8OCB was also investigated at 370 K (isotropic liquid), 350 K(nematic), 330 K (smectic) and 310 K (crystal).
As a spectrum of rotational motion is approximately described by sum of a delta
function (an elastic component) and a
Lorentz function (a quasielastic component), we ﬁrst ﬁtted the spectra with these
two functions. However, the result was notquite. We next tried to ﬁt the data with two
Lorentz functions, which was actually better. The HWHM of the Lorentz function
for narrow component increases with increasing momentum transfer (Q), indicating the narrow component as a diffusive
motion. The diffusion constants were obtained by using the continuous diffusion
model. An Arrhenius plot for the diffusion
constant gives the activation energy 23.5
kJ /mol (Fig. 1). The 8OCB spectra could
also be ﬁtted by two Lorentz functions.
The HWHM of the narrow component wassigniﬁcantly broader than that of 8*OCB,
which means that this diffusive motion of
8OCB is faster than that of 8*OCB. However, the diffusion constants of 8OCB determined in this QENS experiment wereclearly larger than those obtained before
by NMR measurements [4] (Fig. 1). In addition, rotational diffusion constants about
its long axis for 8OCB, obtained by another
NMR measurements [5], are about 10 nsˆ1 at 340 K. This value is in the resolutionwindow of AGNES, so we must have observed this motion. Therefore, the narrowcomponent should be interpreted as a coupled motion of translational diffusive motion and rotation around its long axis.
For the broad component, the activationenergy was determined to be 4.8 kJ/mol by
an Arrhenius plot of the HWHM. This motion may be some internal molecular motion such as rotation of the methyl groups

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or tumbling motion of the alkyl chain.
The rotational diffusion coefﬁcient was estimated to be around 1.2 rad/ps at 350
K. For this broad component, the resultsof 8*OCB and 8OCB are almost same. It
should be added that this motion was observed in the crystalline phase of 8OCB at
310 K as well, while it was not observedin the metastable or the stable crystal for
8*OCB at 270 K.
[1] K. Saito, M. Massalska-Arodz, S.
Ikeuchi, M. Maekawa, J. Sciesinski, E. Sciesinska, J. Mayer, T. Wasiutynski, M. Sorai,
J. Phys.Chem. B, 108 (2004) 5785.
[2] J. Sciesinski, E. Sciesinska, M.
Massalska-Arodz, J. Mol. Struc., 596(2001) 229.
[3] M. Massalska-Arodz, G. Williams, D. K.
Thomas, G. Aldridge, IEEE Trans. Dielectr.
Electr. Insul., 8 (2001) 377.
[4] M. Cifelli, P. J. McDonald, C. A. Veracini,Phys. Chem. Chem. Phys., 6 (2004) 4701.
[5] A. V. Zakharov, Ronald Y. Dong, Phys.
Rev. E 63 (2000) 011704.

Fig. 1. Fig. 1 An Arrhenius plot of the diffusion constant for 8*OCB and 8OCB obtained in this QENS
study, and the translational diffusion constant for
8OCB obtained by NMR measurements (Ref. 4).

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1-1-7

Crystal Structure of Tantalum Oxynitride TaON, a Visible Light Responsive
Photocatalyst
Masatomo Yashima, Yungi Lee*, and Kazunari Domen*
Department of Materials Science and Engineering, Interdisciplinary Graduate School of Scienceand Engineering, Tokyo Institute of Technology, Nagatsuta-cho 4259, Midori-ku, Yokohama-shi,
Kanagawa, 226-8502, Japan; * Department of Chemical System Engineering, School ofEngineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan
Metal oxide photocatalysts have attracted
extensive research for the purposes of solar energy conversion and environmental
remediation. Overall water splitting usinga photocatalyst is an attractive solution forthe supply of clean and recyclable hydrogen energy, while certain photocatalysts
decompose waste materials and hazardous
compounds. Although a large number ofphotocatalysts have been proposed to date,most function only in the ultraviolet (wavelength < 400 nm) region (e.g., TiO2) due tothe inherently large band gap of metal oxides. Metal oxynitrides are candidates forvisible-light responsive photocatalysts, andpromising results have been reported for
TaON, N-doped TiO2, and (Ga1-xZnx)(N1xOx). TaON has been demonstrated to be
responsive to excitation at wavelengths up
to ca. 530 nm, with a suitable band gap (2.3eV) position for overall water splitting. In
the present work, the crystal structure andelectron density of an active TaON photocatalyst sample under visible-light excitation are investigated by neutron diffraction for conﬁrmation of anion ordering,and synchrotron powder diffraction for
high-precision analysis of the crystal structure and electron density. Density functional theory (DFT) is employed for theoretical calculations of the electron density
distribution and partial density of states.
This work was published in Masatomo
Yashima, Yungi Lee and Kazunari Domen,
Crystal Structure and Electron Density of
Tantalum Oxynitride TaON, a Visible Light
Responsive Photocatalyst , Chem. Mater.,
19, [4] 588-593 (2007).
Neutron powder diffraction experiments
were performed using the Kinken pow-

der diffractometer in order to ensure highefﬁciency and high-resolution measurements. The diffractometer, HERMES [2], isinstalled at the JRR-3M Japan Research Reactor of the Japan Atomic Energy Agency(JAEA) in Tokai, Japan and is operated by
the Institute of Materials Research of Tohoku University. Incident neutrons with aﬁxed wavelength of 0.18150 nm were obtained by a vertically focusing (331) Ge
monochromator. Diffraction data were collected at step intervals of 0.1 deg. overa 2 theta range of 8-150 deg. using 150
3He counters set at 1 °intervals. Structural
reﬁnement was performed using the Rietveld analysis program RIETAN-2000 [3].
The peak shape was assumed to be a modiﬁed pseudo-Voigt function with asymmetry. The cut-off value was 7.00 × FWHM
(full-width at half-maximum). The background of each proﬁle was approximatedby a 12-variable polynomial in (2theta)ˆn(n = 0...11). The parameters n were reﬁned simultaneously with the unit cell,structural and proﬁle parameters. The nuclear density of TaON was investigatedby the maximum-entropy method (MEM)with MEM-based pattern ﬁtting (MPF) [4].
The MEM calculations were performed using the computer program PRIMA [4] witha 64 × 64 × 64 pixel unit cell.
All reﬂections in the neutron and synchrotron powder diffraction proﬁles wereindexed as belonging to a monoclinic cell,
indicating a single phase of baddeleyitetype TaON. Rietveld analyses of the neutron and synchrotron diffraction data werethus performed assuming a baddeleyitetype structure. All the occupancy factors
were therefore ﬁxed at unity in the ﬁnal

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reﬁnement. Isotropic harmonic atomic displacement parameters were used for all
atoms. In a preliminary analysis, the atomic
displacement parameters B for the threeatoms were reﬁned independently. However, as the reﬁned atomic displacement
parameter was negative, ﬁnal reﬁnement
was conducted assuming B(Ta) = B(N) =B(O), where B(X) denotes the atomic displacement parameter of X atom. The calculated intensity obtained after ﬁnal reﬁnement was in good agreement with the observed data. The neutron and synchrotron
data sets both indicate that the TaON material has a baddeleyite-type structure (spacegroup, P21/c), with estimated unit cellparameters of a = 0.494941(4) nm, b =0.501662(4) nm, c = 0.516430(2) nm, alpha= 90 °, beta = 99.6107(4) °, gamma = 90 °,and V = 0.126426(2) nmˆ3 (298 K). Occupational ordering of the anions occurs in alternate NTa4 and OTa3 layers normal to the[100] direction. The coordination numbersof Ta, N and O atoms are 7, 4 and 3, respectively. The NTa4 tetrahedron is linked
with four corner-shared NTa4, four edgeshared NTa4, two corner-shared OTa3, andone edge-shared OTa3. The OTa3 triangle
is linked with twelve corner-shared NTa4,
one edge-shared NTa4, three corner-shared
OTa3, and one edge-shared OTa3. These results indicate that the nitrogen atoms preferto be four-coordinated in TaON, while oxygen atoms prefer to have three neighbors.
Figure 1 shows the reﬁned crystal structure, MEM electron density distribution,
MEM nuclear density distribution, and
VASP valence electron density distribution
on the b-c plane of the TaON photocatalyst
over the range 1/4 < x < 3/4. The nuclear
density map shows an atom near the stable
position, and the MEM and valence electron density maps clearly indicate covalent bonding between the Ta and N atoms.
Again, the synchrotron-based electron density distribution (Fig. 1(b)) is in agreementwith the DFT-based valence electron density distribution (Fig. 1(d)). These results
suggest a two-dimensional network consisting of covalent bonds between Ta andN atoms, while the results of Ta-O layer
indicate a two-dimensional network of covalent bonds between Ta and O atoms.
The networks of Ta-N and Ta-O covalentbonds are arranged alternately along the caxis, corresponding to the ordering of NTa4
tetrahedra and OTa3 triangles.
References[1] M. Yashima et al., Chem. Mater. 19(2007) 588.
[2] K. Ohoyama et al., Jpn. J. Appl. Phys. 37(1998) 3319.
[3] F. Izumi and T. Ikeda, Mater. Sci. Forum.
321-324 (2000) 198.
[4] F. Izumi and R. A. Dilanian, Recent Res.
Develop. Phys. 3 (2002) 699.

Fig. 1. (a) Reﬁned crystal structure, (b) electron
density, (c) nuclear density and (d) valence electron
density distributions on the b-c plane of TaON over
the range 1/4 < x < 3/4.

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1-1-8

Diﬀusion Path of Oxide Ions in Apatite-type La9.25Si6.0O25.88
Roushown Ali,*,** Masatomo Yashima,** Yoshitaka Matsushita,* Fujio Izumi,* Shinichi
Kikkawa,*** Takahiro Wakita**Quantum Beam Center, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki
305-0044; **Department of Materials Science and Engineering, Interdisciplinary Graduate
School of Science and Engineering, Tokyo Institute of Technology, 4259 Nagatsuta-cho,
Midori-ku, Yokohama, 226-8502; ***Division of Material Science and Engineering, Graduate
School of Engineering, Hokkaido University, Sapporo 060-8628, Japan
Solid oxides exhibiting high ionic conductivity have been the subject of considerable research interest. In particular, theoxide-ion conductors are useful materials
for fuel cells, catalysts, gas sensors and batteries. The development of improved electrolyte materials for these applications requires a thorough understanding of thecrystal structure and diffusion path of mobile oxide ions, which determine the mechanism of ionic conduction. Lanthanum silicates La10-xSi6O26+delta having apatitetype structure are one of the promisinggroups exhibiting signiﬁcant oxide ion conductivity but the understanding of the conduction mechanism in this structure remains subject to uncertainties. Here, wehave investigated the crystal structure anddiffusion pathway of oxide ions in apatitetype compound La9.25Si6.0O25.88 at 1558
degrees Celsius.
The neutron powder diffraction data werecollected at 1558 degrees Celsius on HERMES installed at the JRR-3M reactor. Incident neutron beams with a ﬁxed wavelength of 0.18265 nm were obtained by avertically focusing (331) Ge monochromator. A furnace [1] with an MoSi2 heater
was used to heat the sample and the sample temperature was maintained within +1.5 degrees Celsius. during the measurement. The resulting diffraction data wereanalyzed by the Rietveld method withRIETAN-FP [2] and whole-pattern ﬁtting
approach based on the maximum-entropy
method (MPF) [3]. The MEM calculation
was done with the unit cell divided into 100
X 100 X 80 pixels and whole-pattern ﬁtting
using RIETAN-FP.

The Rietveld reﬁnement was performed
with hexagonal space group P63/m
through the neutron powder diffraction
data measured at 1558 degrees Celsius.
Attempts to reﬁne the structure considering an interstitial oxygen atom site were
not successful, so the reﬁnement were
performed without interstitial site. The
calculated pattern agreed well with thatof observed pattern. The reliability values
obtained from the reﬁnement were Rwp= 2.15 %, Rp = 1.67 %, RI = 1.20 % RF
= 0.72 % and S = 2.05. The reﬁnement
was carried out with anisotropic thermal
displacement parameters for all the cations
and anions. The thermal displacement
parameters of oxygen O3 atoms showedstrong anisotropic along the a-axis withlarge U11 value (0.00123(3) nmˆ2) whilethat of O4 showed stronger anisotropic
along the c-axis with larger U33 value(0.0025(1) nmˆ2). The structure consists of
six isolated [SiO4] tetrahedra containing
three kinds of oxygen atoms (O1, O2, O3).
The oxygen atoms O3 and O4 displayedlarge displacement parameters, suggesting directionality in the movements ofoxide ions around their stable positions.
The probability densities of O4 atoms wereconnected with that of nearest-neighbor O4
atoms, indicating diffusion along a pathway parallel to the c axis. The O4 atoms
migrated linearly to the nearest-neighbor
O4 and followed one-dimensional tunnel
extending along the c axis of the hexagonal
P63/m framework. On the other hand,the probability densities of O3 atoms
were largely distributed perpendicular tothe c axis. The main diffusion pathway

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involved one-dimensional migration along
the hexagonal channels of the apatitetype structure. The directionality in the
movements of oxide ion O3 also suggests
another migration pathway perpendicular
to the c-axis.
References[1] M. Yashima, J. Am. Ceram. Soc. 85(2002) 2925.
[2] F. Izumi and K. Momma. In Proc. XX
Conf. Appl. Crystallogr., Solid State Pherich, 2007. Trans Tech Publicanom., Z
tions. in press.
[3] F. Izumi and R. A. Dilanian, Recent Res.
Dev. Phys., 3 (2002) 699.

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1-1-9Structural investigation of the cubic perovskite-type doped lanthanum cobaltite
La0.6Sr0.4CoO3-delta at 1258 degrees Celsius, - Possible diﬀusion path of oxygenions in an electrode material Masatomo Yashima and Takayuki Tsuji
Department of Materials Science and Engineering, Interdisciplinary Graduate School of Scienceand Engineering, Tokyo Institute of Technology, 4259 Nagatsuta-cho, Midori-ku, Yokohama-shi
226-8502, Japan(1) Introduction
Perovskite-structured oxides that exhibit
high ionic conductivity have attracted considerable attention due to their various applications in solid oxide fuel cells (SOFCs),
batteries, catalysts and oxygen sensors.
The development of better oxygen-ion andmixed conductors requires a better understanding of the diffusion paths andstructural disorder of mobile oxygen ionsat high temperatures at which the materials work efﬁciently. The lanthanum
strontium cobaltites, La1-xSrxCoO3-delta,
which have a perovskite-type structure,are promising electrode materials for the
doped lanthanum gallate electrolyte in
SOFCs. The crystal structure of rhombohedral R-3c La1-xSrxCoO3-delta has been
the subject of a number of previous investigations. However, far less attention
has been paid to the high-temperature cubic La1-xSrxCoO3-delta phase. The purpose of the present study is to investigate the crystal structure and structural
disorder of the cubic Pm-3m perovskitetype La0.6Sr0.4CoO3-delta at 1258 degrees
Celsius. This work was published in M.
Yashima and T. Tsuji, Structural investigation of the cubic perovskite-type doped
lanthanum cobaltite La0.6Sr0.4CoO3-delta
at 1531 K: possible diffusion path of oxygen ions in an electrode material , J. Appl.
Crystallogr., 40, [6] 1166-1168 (2007).
(2) Experiments and data processing
La0.6Sr0.4CoO3-delta specimens wereprepared through solid-state reactions by
the Mitsubishi Materials Co. Neutron powder diffraction data were collected in air us-

ing HERMES, a diffractometer with a 150multi-detector system, at room temperature and at 1258 degrees Celsius (Ohoyama
et al., 1996). The HERMES diffractometer islocated at the T1-3 port of the JRR-3M research reactor of the Japan Atomic Energy
Agency at Tokai, Japan. The powder patterns were measured in the range from twotheta = 5 degrees to 155 degrees. The wavelength of the incident neutrons was 0.18207
nm. The sample temperature was kept constant during the data collection at 1258.2degrees Celsius (+1.4 degrees Celsius, -0.8 degrees Celsius) using a furnace with MoSi2
heaters (Yashima, 2002).
The diffraction data obtained at 1258 degrees Celsius were analyzed by a combination of Rietveld analysis, the maximumentropy method (MEM) and MEM-based
pattern ﬁtting (MPF) (Izumi & Dilanian,2002). The computer programs RIETAN2000 (Izumi & Ikeda, 2000), PRIMA (Izumi& Dilanian, 2002) and VESTA (Momma& Izumi, 2006) were utilized for the Rietveld and MPF analyses, MEM calculations and visualization of crystal structure
and the nuclear-density distribution, respectively. The coherent scattering lengths(bc) adopted for Rietveld reﬁnement were
8.24 fm for La, 7.02 fm for Sr, 2.49 fm for Co
and 5.803 fm for O.
(3) Results and discussion
Neutron-diffraction data forLa0.6Sr0.4CoO3-delta at room temperature indicated that the specimen consistedof a single phase of the rhombohedral
La0.6Sr0.4CoO3-delta. All the peaksin the neutron diffraction pattern ofActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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La0.6Sr0.4CoO3-delta at 1258 degrees Celsius were indexed by the cubic perovskitetype structure with Pm-3m symmetry,
indicating phase transformation from a
low-temperature rhombohedral to a hightemperature cubic phase. Rietveld analysis
was performed using the diffraction datataken at 1258 degrees Celsius in the twotheta range of 20 degrees to 153 degrees bya cubic perovskite-type structure. La and Sr
atoms were placed at the special position
1b 1/2, 1/2, 1/2 of the Pm-3m symmetry.
Co and O atoms were placed at the 1a 0,
0, 0 and 3d 1/2, 0, 0 sites, respectively.
Isotropic and anisotropic atomic displacement parameters were used for the cations
and anions, respectively. The calculated
proﬁle agreed well with the observed one.
The atomic displacement parameters of
the O atom exhibited large anisotropy,
which reﬂects the rotational motion of
O atoms in the rigid CoO6 octahedron.
Similar anisotropy has been observed inother cubic perovskite-type compounds.
The equivalent isotropic displacement
parameter of O atom is larger than those of
cations, suggesting the higher diffusivityof O atoms. The occupancy factor of the
O atom at the 3d site was estimated to be
0.886(6), indicating an oxygen deﬁciency
of delta =0.34(2) in La0.6Sr0.4CoO3-delta
at 1258 degrees Celsius. The averaged
valence of the Co cations was estimatedto be 2.72 at 1258 degrees Celsius, whichis consistent with the calculated bondvalence sum value of 2.8. Here, the averagevalue of the bond valence parameter of
1.698 was used for the calculation.
MEM-based pattern ﬁtting (MPF) analysis was conducted using diffraction datain the two theta range from 20 degrees to
153 degrees, corresponding to d > 0.107
nm (d: spacing of lattice planes), with thestructure factors obtained from Rietveld
analysis. A total of 16 structure factors
were obtained. The 100 reﬂection appearing at the lowest two theta position (ca.
26.7 degrees) was included, since this peakprovides information on the disorderedarrangements of oxygen ions. The MEM

calculations were performed with the unit
cell divided into 64 X 64 X 64 pixels. The R
factors for the Bragg intensities, RI and forthe structure factors, RF were improved
from 2.33 % in the Rietveld analysis to1.71 % in the MPF, and from 1.72 % to1.25 %, respectively. The nuclear-density
map reveals that the oxygen ions in the
cubic Pm-3m La0.6Sr0.4CoO3-delta exhibit
a large thermal motion perpendicular to
the Co-O bond, corresponding to large
anisotropy of the atomic displacement
parameters. The diffusion path does notfollow the edge of the CoO6 octahedron
shown as straight lines, but displays an
arc shape away from the Co cation. Itshould be noted that the nuclear density of O atoms in La0.6Sr0.4CoO3-delta
did not connect with that of nearest
neighbor O atoms. On the contrary, the(La0.8Sr0.2)(Ga0.8Mg0.15Co0.05)O2.8
perovskite exhibited connected diffusion paths. This strongly suggeststhat the diffusivity of oxygen ions in
La0.6Sr0.4CoO3-delta is lower than that in(La0.8Sr0.2)(Ga0.8Mg0.15Co0.05)O2.8.

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1-1-10Low-Energy Phonon Anomaly of CeOs4 Sb12
K. Iwasa1 , S. Itobe1 , C. Yang1 , Y. Murakami1 , M. Kohgi2 , H. Sugawara3 , H. Sato2
Tohoku Univ.1 , Tokyo Metropolitan Univ.2 , The Univ. of Tokushima3
The rare-earth ﬁlled skutterudites
RT4 X12 (R = rare earth, T = transition
metal, X = pnictogen) have been studiedin terms of the anomalously anharmonic
lattice properties, as well as the various
strongly correlated electron phenomena
involving 4 f electrons. The ﬁlled ions arelocated within the icosahedral X cage, andvibrate with large amplitude detected as
the large Debye-Waller factors. Ultrasonicmeasurements of PrOs4 Sb12 revealed
dispersion of elastic constants indicativeof anomalous Pr-ion motion within the
Sb cage (T. Goto et al.: PRB 69 (2004)
180511). Recent inelastic x-ray scatteringexperiment of Sm-based compounds (S.
Tsutsui et al.: Physica B 383 (2006) 142) andinelastic neutron scattering experimentof CeRu4 Sb12 (C. H. Lee et al.: JPSJ 75(2006) 123602) revealed low frequency ﬂat
phonon branches corresponding to the
motion of ﬁlled atoms. We have reported
the anomalous softening of phonon due to
Pr vibration with decrease of temperatureand the possible electron-phonon interaction in PrOs4 Sb12 and PrRu4 Sb12 (K. Iwasa
et al.: Physica B 378-380 (2006) 194, J. Phys.
Conference Series 92 (2007) 012122). In thepresent study, we have investigated thelow-energy phonon spectra of CeOs4 Sb12
using the triple-axis spectrometers TOPAN(6G) and HER (C1-1).
The ﬁgure shows phonon spectra of
CeOs4 Sb12 measured at the reciprocal lattice point Q = (0 3 3). It shows distinct decrease of excitation energy by 18% with decreasing temperature from 300 down to 15
K. This softening mode was conﬁrmed tobe less dispersive like an optical mode. We
measured phonon spectra also at Q = (6 -0.4
-0.4), and it also exhibits softening by 10%.
The energy region of this mode as wellas the softening indicate that this phonon
is composed of the vibration of the Ce

atoms within the icosahedral Sb cage. The
presence of such anharmonic low-energy
phonon in the three measured compounds
suggests that it is common feature in therare-earth ﬁlled skutterudite. We will continue the study to reveal the mechanism of
the softening behavior, which may be mode
coupling effect or the electron-phonon interaction involving the anomalous rareearth vibration mode.

Fig. 1. Temperature dependence of the phonon
spectra at Q = (0 3 3) of CeOs4 Sb12 .

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1-1-11

Observation of spin dynamics in Shastry- Shutherland lattice TbB4
K. Ohoyama, T. Matsumura(A), D. Okuyama(A), F. Iga(B), S. Michimura(B)IMR, Tohoku Univ., Faculty Science, Tohoku Univ.(A), ADSM, Hiroshima Univ.(B)(middle ﬁgure). On the other hand below TN2, the excitation rapidly change
the position to about 2meV and increases
with decreasing temperature (bottom ﬁgure). This suggests that some kind of softening of excitation occurs above TN2. Furthermore, since the excitation energy nearTN2 is smaller than the thermal energy,
some quasi-degeneracy may play an important role for the magnetic properties in
TbB4. To clarify the bahaviour of the lowlying 4f states around TN2, higher resolution experiments are in progress.
6G 3axis kf=2.6699A-1 B-30-S-PG-30-B'60.1K
40.0K
36.3K
30.3K
28.3K

CNT/ 3000k

600

400

200

CNT/300K

0
600

26.3K
24.2K
22.1K

400

200

0
600
CNT/300K

Rare earth compounds RB4 have attracted our interests because the geometrical alignment of the rare earth ions in
the c-plane is equivalent with that of
the Shastry-Sutherland lattice in whichmagnetic frustration is theoretically predicted. Of this system, TbB4 reveals successive magnetic transitions at TN1=42.1K
and TN2=21.7K. An important characteristic point of TbB4 is that, in magnetization process for B//[001], TbB4 shows
9-steps metamagnetic transitions between
15T<H<30T below TN2, even though
the magnetic structure under B=0T is an
Heisenberg type antiferromagnetic one: all
the magnetic moments below TN2 lies in
the c-axis. The metamagnetic transitions in
a Heisenberg-type magnet imply some unknown magnetic properties in RB4.
To understand magnetic properties in
TbB4, it is indispensable to understand4f ground state and low-lying 4f levels.
Therefore, we are systematically investigating magnetic excitations in TbB4 underzero magnetic ﬁeld. In 2007, we performed
neutron inelastic scattering experiments ona single crystalline sample of Tb11B4 on 6G
and T1-2, and found some characteristic behaviour of spin dynamics around the transition temperatures. The collimation condition were B-30-S-PG ﬁlter-30-B to obtainhigher resolution. The constant Ef mode
was selected with kf=2.67A-1.
Fig.1 shows the temperature dependence
of energy spectra of TbB4 observed on 6G
at the (100) reciprocal lattice point whichcorresponds to the magnetic zone centre.
As shown in the ﬁgure, a magnetic excitation was observed at about 3meV at T=60K;
the excitation energy decreases down to
1.5meV with decreasing temperature (topﬁgure); the excitation can not be distinguished from the elastic scattering aroundTN2 under present resolution condition

20.1K
17.9K

400

200

0
-1

0

1

2

3

4

Energy Transfer (meV)Fig. 1. Energy spectra of TbB4 observed on 6G atseveral temperatures at the (100) reciprocal point.
Top: T>TN2, Middle: near TN2, Bottom: T<TN2

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1-1-12Crystal Structure of Chemically Modiﬁed Layered Cobaltates
Yuzuru Miyazaki, Dai Igarashi and Tsuyoshi Kajitani
Department of Applied Physics, Graduate School of Engineering, Tohoku University
Recently, a ﬁrst-order structural transition has been discovered for the gammaNaxCoO2 (x˜0.58) sample at the temperature range from T1 = 236 K to T2 =288
K. Above T2, the compound possesses anidentical structure to well known gammaNaxCoO2, in which the Na1 and Na2
atoms are randomly distributed. In thisstudy, we have determined the crystal
structure of the compound between T1
and T2. Neutron powder diffraction (ND)
data were collected at several temperatures by the use of HERMES diffractometer. The ND data were analyzed using theRietveld reﬁnement program RIETAN2000.
According to the electron diffraction pattern taken at 248 K, the compound has anorder ’sqrt’7 x ’sqrt’7 ordered superstructure with the space group of P63/m. In Fig.
1, we show the revealed crystal structureof Na0.58CoO2 at 300 K and 240 K, projected parallel to the c-axis. The structure
at 300 K is found to be isostructural to thepotassium analogue, K4Co7O14, reported
by Blangero et al[1]. At 240 K, the each single Co and O site split into two and threesites with different z-coordinations, respectively. This site-splitting yields an undulated CoO2 conduction plane with inequivalent Co-O lengths. The observed anomaly
in resistivity and magnetic susceptibility at
T2 can be understood by such a change inthe bond lengths of the electronic conduction paths.
[1] M. Blangero et al, Inorg. Chem. 44 (2005)
9299.

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JAEA-Review 2011-050

1-1-13Structural disorder of cubic Ce0.5Zr0.5O2 solid solution
Takahiro Wakita(A), Masatomo Yashima(A), Yoshitaka Matsushita(B), Takafumi
Komatsu(A), Yong Phat(A), and Takashi Ohta(A)(A)Department of Materials Science and Engineering, Interdisciplinary Graduate School of
Science and Engineering, Tokyo Institute of Technology (B) Quantum Beam Center, National
Institute for Materials Science
The crystal structure of the CeO2-ZrO2
solid solutions has been investigated by
Yashima et al. [1,2]. They reported the existence of three metastable tetragonal formsof t, t and t . The three tetragonal forms
belong to the P42/nmc space group. However, structural disorder and diffusion pathof oxygen ions in Ce0.5Zr0.5O2 solid solution remain poorly understood. In thisstudy, we demonstrate that there is considerable positional disorder of the oxygenions in Ce0.5Zr0.5O2 solid solution. Hightemperature neutron powder diffracrtion
data at 1832 K are utilized because of therelatively high contributions to the structural disorder of oxygen ions, and it is easy
to compare with CeO2, which has a cubic
structure.
Ce0.5Zr0.5O2 powders were preparedby a coprecipitation route. Ce0.5Zr0.5O2
powders were pressed into pellets. CeO2
powders were prepared by a neutralization method. The powders were pressed
into pellets. These pellets were used forhigh-temperature neutron diffraction measurements. Neutron diffraction measurements were performed in air with a 150detector system, HERMES [3], installed at
the JRR-3M reactor in Japan Atomic Energy Agency, Tokai, Japan. Neutrons withwavelength 1.8143 angstrom and 1.8207
angstrom were obtained by the (311) reﬂection of a Ge monochromator. Diffraction data were collected in air at 1832
K and at 1826 K. A furnace with MoSi2
heaters [4] was placed on the sample table, and used for neutron diffraction measurements at high temperatures. The experimental data were analyzed by a combination of Rietveld analysis, the maximumentropy method (MEM) and MEM-based

pattern ﬁtting (MPF). Computer programs
RIETAN-2000 [5], PRIMA [6] and VESTA[7] were utilized for the Rietveld and
MPF analyses, MEM calculation and visualization of crystal structure and nucleardensity distribution, respectively.
Rietveld analysis of the neutron diffraction data of Ce0.5Zr0.5O2 at 1832 K andCeO2 at 1826 K was carried out based ona cubic ﬂuorite-type structure with Fm-3m
space group. The calculated proﬁle is ingood agreement with the observed data.
Figures 1(a) and (b) show nuclear density contour maps on the (110) plane forCe0.5Zr0.5O2 and CeO2 at 1832 K and 1826
K, respectively. The results reveal that theoxygen ions in Ce0.5Zr0.5O2 show complicated disorder and are spread over awide area compared with CeO2 (Fig.1). The
oxygen ions show a shift to the <111>directions (Fig.1). Possible diffusion pathsof the oxygen ions can be seen along the<100> and <110> directions (see dottedarrows (A) and (B) in Figs. 1(a) and (b)).
The spatial distribution of oxygen ions in
Ce0.5Zr0.5O2 is greater than that of CeO2.
The greater degree of positional disorder in
Ce0.5Zr0.5O2 is responsible for higher diffusivity of the oxygen ions.
References[1] M. Yashima et al., J. Am. Ceram. Soc. 76(1993) 2865.
[2] M. Yashima et al., Appl. Phys. Lett. 72(1998) 182.
[3] K. Ohoyama et al., Jpn. J. Appl. Phys. 37(1998) 3319.
[4] M. Yashima, J. Am. Ceram. Soc. 85(2002) 2925.
[5] F. Izumi and T. Ikeda, Mater. Sci. Forum.
321-324 (2000) 198.

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JAEA-Review 2011-050[6] F. Izumi and R. A. Dilanian, Recent Res.
Develop. Phys. 3 (2002) 699.
[7] K. Momma and F. Izumi, Commission
on Crystallogr. Comput., IUCr Newslett. 7(2006) 106.

Fig. 1. Nuclear density distributions on the (110)planes of (a) Ce0.5Zr0.5O2 and (b) CeO2 with black
contours in the range from 0.7 to 5.0 fm / angstrom3(0.5 fm / angstrom3 step) at 1832 K and 1826 K, respectively.

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JAEA-Review 2011-050

1-1-14Magnetic structure in CuFeP66
Miwako Takahashi1 , Ejaz Ahmed1 ,Ken-ichi Ohshima1 and Yukio Noda2
Inst. of Mat. Sci., Univ. of Tsukuba1 , IMRAM, Tohoku Univ.2
dependence of intensity and position of 110
magnetic peak. Below TC , peak position
show gradual shift with increasing intensity and takes almost constant value below
TN . These results indicate strong correlation between magnetic and atomic structures.
[1] M. Takahashi, E. Ahmed, A. K. Das, Y.
Fujii, H. Iwasaki and K. Ohshima : J. Alloys. Compd. in print.
8

intensity at 0.5 0.5 0 (counts/10sec)(a)

50
CuFePt6quenched
0.5 0.5 0
110

7
6

45
40

5

35

4

30

3

25

2

T N2

T N1

1

Intensity at 110 (counts/10sec)

20

TC

15
0

50

100

150

200

250

Temperature (K)

(b)

10.4

CuFePt6 annealed(100)
peak intensity
omega position
guid to eyeomega (degree)

10.3

400

300

200

10.2

100

peak intensity (counts/5sec)

CuFePt6 is one of the newly foundternary alloys CuMPt6 (M; 3d elements).
It has fcc fundamental structure andforms Cu3 Au-type ordered structure below1313 K. Magnetic susceptibility shows different behavior for the alloys with disordered and ordered structures, indicatingstrong relation between magnetic properties and atomic ordered structures. Temperature dependence of magnetic susceptibility shows ferromagnetic transition for
the alloys in both ordered and disorderedstate: at TC = 200 K for the ordered state
and at TC = 185 K for the disorderedstate. Below TC , susceptibility under FC
and ZFC processes shows different behavior. The former shows normal ferromagnetic behavior but the latter shows successive antiferromagnetic-like transitions at
TN = 100 K for the ordered state and at
TN1 = 90 K and TN1 = 30 K for the disordered state. On the other hand, variationof magnetization at 5 K shows typical ferromagnetic curves with little hysteresis forthe alloys in both ordered and disorderedstates.
The magnetic structure of the alloy withboth ordered and disordered state has beenstudied with a four-circle diffractometer,
FONDER at T2-2. Figure 1(a) shows temperature dependence of the intensities ofmagnetic scattering in the alloy with disordered state. magnetic intensities appear at
1 1 0 (X-point of fcc) below TC , and at 1/2
1/2 0 below TN1 . These magnetic intensities begin to decrease below TN2 ; measurement at lower temperature is required forthe study of magnetic phase below TN2 .
In the alloy with ordered state, magnetic
scattering appears at 1 1 0 (Γ-point of sc) below TC and at 1/2 1/2 0 (M-point of sc) below TN , the same point as in the alloy withdisordered state but with much stronger intensities. Figure 1(b) shows temperature

10.1

TN
50

100

0
150

Temperature (K)

200

TC

Fig. 1. (a)Temperature dependence of the intensities
at 1/2 1/2 0 (closed circles) and 1 1 0 (open circles)
in disordered state. (b) Temperature dependenceof peak position (closed circles) and peak intensity(open circles) at 1 1 0 in ordered state.

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JAEA-Review 2011-050

1-1-15Magnetic excitation in CuFeP66
Miwako Takahashi1 , Ejaz Ahmed1 ,Ken-ichi Ohshima1 and Naoto Matsura2
Inst. of Mat. Sci., Univ. of Tsukuba1 , ISSP, Univ. of Tokyo2
below ΔE < 4 meV show no dispersion
and do not appear at the equivalent points.
Inelastic intensities along 0kk and 1kk at
ΔE = 2 and 3 meV are shown in Fig.1(b).
At k = 0.45 and 0.65 of 0kk line, inelastic
peaks with both ΔE = 2 and 3 meV appear, though no clear peaks are observed
along the symmetrical line of 1kk. The inelastic peaks are found to persist far above
TN . Further experiments should be necessary to clarify the origin of the magnetic excitation.
[1] M. Takahashi, et al : J. Alloys. Compd.
in print.
(a)< 4 meV> 4meV

011(Γ)
1.0
1kk scan0kk
0.5
0 1/2 1/2 (M )1 1/2 1/2 (M )0kk scan

0.0
-0.5

0.0

0.5

1.0

h00

0 k k scan; Intensity / 1600K (~ 8min.)

(b)

400

250

CuFePt6
furnace cooled HKK
14.7Ef open -80-S-PG-80-open
7.3 K

300

150

0 k k scan (3 meV)1 k k scan (3 meV)0 k k scan (2 meV)

200

200

100

100
50

0

1 k k scan; Intensity / 1600K (~ 8min.)

Ternary alloy CuFePt6 shows anomalous
magnetic behavior[1] . It has fcc fundamental structure and forms Cu3 Au-typeordered structure below 1313 K. The alloys with both ordered and disorderedstates undergo ferromagnetic and antiferromagnetic transitions, though the transitions take place at different temperaturesin the different ordered states. Temperature dependence of magnetic susceptibility ﬁrst shows ferromagnetic transition at
TC = 200 K for the ordered state andat TC = 185 K for the disordered state.
Below TC , susceptibility under FC andZFC processes shows different behavior.
The former shows normal ferromagnetic
behavior but the latter shows successive
antiferromagnetic-like transitions at TN =100 K for the ordered state and at TN1 =90 K and TN1 = 30 K for the disorderedstate. Magnetic diffraction under zeromagnetic ﬁeld shows magnetic scattering
at 110 (X-point in fcc disordered state andΓ-point in sc ordered state) below TC , and
1/2 1/2 0 (M-point in sc ordered state)
below TN and TN1 . The results indicatecompetitive existence of the two types ofmagnetic structures in the alloy and themagnetic phase is sensitively dependent on
the magnetic ﬁeld and the atomic arrangement. To investigate dynamical ﬂuctuationin the ferromagnetic and antiferromagnetic
structures, inelastic neutron scattering was
performed at the triple-axis-spectrometer
PONTA.
Figure 1(a) shows observed inelastic
peaks with ΔE below 4 meV (black closed
circles) and above 4 meV (open circles) at
7 K on (hkk ) plane in the alloy with ordered state. In the ﬁgure, green, blue andred closed circles represent 000 (Γ-point),
011 (Γ-point in ordered and X-point in disordered state), and 0 1/2 1/2 (M-point inordered state), respectively. Inelastic peaks

0
0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

1.1

1.2

k in 0 k k

Fig. 1. (a)Inelastic peaks with ΔE below and above
4 meV (closed and open black circles) at 7 K. (b) Inelastic intensities along 0kk(red circles) and 1kk(bluecircles) at ΔE = 2 (open circles) and 3 meV (closed
circles).

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1-1-16

Neutron scattering study of phonon dynamics on La3Pd20Ge6
C. H. Lee(A), H. Yoshizawa(B), I. Hase(A), Y. Nemoto(C) and T. Goto(C)(A) AIST, (B) ISSP, (C) Niigata Univ.
A large vibration of an atom in an
oversized atomic cage, so called rattling,
has attracted great interest since it canbe the origin of exotic physical properties. La3Pd20Ge6 is one of those compounds that have large atomic cages ﬁlledwith La guest atoms. Ultrasonic measurements show that the elastic constant C44 of
La3Pd20Ge6 exhibits a Debye-type dispersion around T = 20K [1]. It is proposed thatthe phenomenon is originated from the rattling motion of La atoms, but there is still
no direct evidence. Rather, the feature of arattling motion is still controversial. In thepresent work, thus, we study phonon dynamics of La3Pd20Ge6 by inelastic neutron
scattering and try to understand the reasonof the Debye-type dispersion as well as thenature of rattling.
Neutron scattering measurements werecarried out using the triple-axis spectrometer, TOPAN, GPTAS and HER, at the
JRR-3 reactor of JAEA at Tokai. The ﬁnal neutron energy was ﬁxed at Ef = 14.8
meV or 5.4 meV using a pyrolytic graphite
monochromator and an analyzer. The sequences of the horizontal collimators were40’-40’-S-40’-40’, 40’-60’-S-60’-60’, open-S80’-80’ or open-S-40’-40’, where S denotes
the sample position. Total sample vomule
of La3Pd20Ge6 single crystals used for themeasurements was about 1.3cc.
Fig. 1 shows the phonon dispersion curveof La3Pd20Ge6 with propagation vector of[100]. The optical phonon mode observed
at E = 1 meV around zone center corresponds to a guest mode, in which La atoms
vibrate largely. Around q=(0.08,0,0), theguest mode shows anti-crossing behavior
with acoustic phonon mode as other cagecompounds[2-4]. Characteristically, theguest mode is quite dispersive, different
with other cage compounds where guest
modes are almost dispersionless. This sug-gests that an interaction between La-La
atoms exists. Temperature dependence ofthe guest phonon energy exhibits hardening below T = 50 K, indicating strong anharmonicity. The relationship between thehardening and the Debye-type dispersion
observed by ultrasound measurements isnow under consideration.
[1] T. Goto et al., Phys. Rev. B 70 (2004)
184126[2] C. H. Lee et al., J. Phys. Soc. Jpn. 75,(2006) 123602[3] C. H. Lee et al., J. Phys.: Conf. Ser. 92,(2007) 12169[4] C. H. Lee et al., J. Phys. Soc. Jpn. Suppl.
(2008) in press

Fig. 1. Phonon dispersion curves of longitudinalphonon modes with propagation vector [100] in
La3Pd20Ge6.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 441

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JAEA-Review 2011-050

1-1-17

Lattice dynamics of NaNbO3
I. Tomeno(A), Y. Tsunoda(B), M. Nishi(C), M. Matsuura(C), K. Oka(D)(A)Faculty of Education and Human Studies, Akita Univ., (B)School of Science andEngineering, Waseda Univ., (C)ISSP, Univ. of Tokyo, (D)Nanoelectrics Research Institute,
AIST
References[1] C. N. W. Darlington and K. S. Knight,
Physica B266, 368 (1999).
[2] W. Zhong and D. Vanderbilt, Phys. Rev.
Lett. 74, 2587 (1995).
[3] F. Denoyer, R. Comes, and M.Lambert,
Acta Cryst. A27, 414 (1971).
NaNbO3

T = 970 K Q=(H, 4-H, 0)
M-point

ΔE =
8 meV

Intensity (arb. units)

Sodium niobate NaNbO3 exhibits acomplex sequence of structural phase transitions as a function of temperature.[1]Above 913 K, NaNbO3 has a simple cubic
perovskite structure. Below this temperature, there are at least six phases. Antiferrodistortive (AFD), antiferroelectric (AF),and ferroelectric (FE) phases have been
identiﬁed in NaNbO3. The complexity ofthe phase transitions suggests the existenceof competing structural instabilities in cubic NaNbO3.[2] We studied the lattice dynamics of cubic NaNbO3. Inelastic neutron scattering measurements were performed using the triple-axis spectrometer
T-11 (HQR) at JRR-3M.
Figure shows constant-E scans for the [1,1, 0] direction polarized along the [1, -1, 0]
direction determined at 970K. In contrast,
constant-E scans for the same direction polarized along the [0, 0, 1] showed that theTA phonon energy is approximately 8 meVat the M point. This indicates that the Mpoint TA phonons with polarization along[1, -1, 0] soften signiﬁcantly in the cubic
phase. Furthermore, we found out the softening of the R-point TA phonons. Softeningof these zone-boundary phonons (the M3
and R25 modes) is interpreted by the instability of rotational modes of oxygen octahedra. In addition, preliminary experiments
show the softening of long-wavelength TO
phonons for the [1, 1, 0] direction polarizedalong the [0, 0, 1] direction. Present resultsroughly explain the diffuse X-ray scattering
data in the cubic phase.[3] The complicatedsituation of soft modes at zone-center andzone-boundaries seems related with the existence of the sequence of phase transitions
below 913 K. Further experiments are necessary to investigate phonon dispersion relations in cubic NaNbO3.

6 meV

4 meV

2 meV

1.3

1.4

1.5

1.6

1.7

H (r.l.u.)

Fig. 1. Constant-E scans around the zone-boundary
M point measured at 970 K.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-1-18

Crystal Structure of Mg-doped apatite-type Ionic Conductor
Y. Matsushita1 , T. Wakita2 , H. Yoshioka3 , M. Yashima2 , and F. Izumi1
1 Quantum Beam Center, National Institute for Materials Science
2 Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology
3 Hyogo Prefectural Institute of Technology
thermal displacement parameters for all
the lanthanum sites and the oxygen sites.
The ﬁnal convergent indexes were Rwp =3.68 %, Rp = 2.67 %, RR = 5.04 %, Re =0.75 %, RI = 1.08 %, and RF = 0.46 %.
The obtained cell parameters from the Rietveld analysis were a = 0.97384(3) nm, andc = 0.72140(2) nm. On the Rietveld reﬁnement process, the interstitial oxygen positions were not able to be clearly observed.
However, the oxygens may locate aroundthe La2 site from crystallochemical point ofview.
References[1] S. Nakayama et al.: J. Mater. Chem. 5 (1995)
1801.
[2] S. Nakayama et al.: Chem. Lett. 24 (1995)
431.
[3] H. Yoshioka et al.: Chem. Lett. 33 (2004) 392.
[4] F. Izumi and T. Ikeda: Mater. Sci. Forum
321-324 (2000) 198.
[5] F. Izumi and R. A. Dilanian: Recent Res.
Develop. Phys. 3 (2002) 699.
10000080000

Intensity (counts)

Oxygen-ionic conductors are very important materials for various kinds of applications such as fuel cells and oxygen-gas
sensors. In 1995, Nakayama found new
type of oxygen-ionic conductor; Ln-Si-O
apatites (Ln = Lanthanoids). [1] [2] These
compounds show better oxygen ionic conductivity in middle range of temperaturecompared with other famous oxygen-ionic
conductors (ZrO2 and/or CeO2 -based materials). Recently, Yoshioka reported that
Mg-doped apatites show the best ionic conduction. [3] However, in all of the apatite system, details of mechanism of ionic
conduction are still under question. In
this study, we carried out powder neutrondiffraction technique to understand crystallographic details of Mg-doped Apatitetype ionic conductor.
The Mg-doped apatite-type sample
was prepared by sol-gel method.
[3]
The chemical composition of the sample,
La9.7 (Si5.7 Mg0.3 )O26.3 , was determinedby inductively coupled plasma measurements.
The neutron powder-diffraction measurement at room temperature, was carriedout using IMR-HERMES diffactmetor (T13), installed in the JRR-3M reactor. The
wavelength of neutron was 0.18265 nm,
which was vertically focused by a (331) Ge
monochromator. The resulting diffraction
data were analyzed by the Rietveld methodwith RIETAN-FP [4] and whole-pattern ﬁtting approach based on the maximumentropy method (MPF) [5].
The Rietveld reﬁnement was performed
with neutron powder diffraction data of
La9.7 (Si5.7 Mg0.3 )O26.3 on the basis of hexagonal P63 /m. The calculated pattern agreed
well with that of observed pattern. The reﬁnement was carried out with anisotropic

60000

40000

20000

0

10

20

30

40

50

60

70

80

90

100

110

120

130

140

150

2q (° )

Fig. 1.
Powder neutron diffraction proﬁle ofLa9.7 (Si5.7 Mg0.3 )O26.3 .

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-1-19Crystal structure and ionic conductivity of Ga system oxides for solid electrolyte offuel cell
Yasushi Idemoto, Tomomasa Sugiyama and Naoto Kitamura
Tokyo University of Science
Gallate-based oxides are regarded aspromising candidates for the electrolyte of
SOFC, because of their high conductivities
and high chemical stabilities. In the oxides,
partial substitution of aliovalent cations
introduces oxygen vacancies and/or protons, and results in signiﬁcant oxide ion
and/or proton conduction above 500 K.
Thus, it is important to clarify their crystal
structures and nuclear densities of theoxide ion and the protons at elevated temperature. Due to the difﬁculty in structural
analysis on such light atoms, however,there are not enough knowledge on them.
In order to make these clearer, we focusedon La0.8Sr0.2Ga0.8Mg0.2O3-d (LSGM)
and La0.8Sr0.2Ga0.8Mg0.115Co0.085O3-d(LSGMC) as oxide ion conductor andLa0.9Ba1.1GaO4 (LBG) as proton conductor, and investigated them with neutron
diffraction measurements.
We obtained LSGM and LSGMC powders by heat-treating precursors preparedby AGC SEIMI CHEMICAL CO., LTD. LBG
was synthesized with solid-state reaction
using each oxide or carbonate as a starting material. As for the products, we characterized their phases by XRD, compositions by EDX, and oxygen nonstoichiometry by microbalance. Conductivity measurements were also performed at elevatedtemperatures. In order to clarify the crystal structures, neutron diffraction patterns
were measured using HERMES of IMR at
the JRR-3M, and these patterns were analyzed with the Rietan-2000. The measurements were performed at 298˜680 K. The
nuclear densities were also estimated basedon MEM using the PRIMA

gle phase of the perovskite-type structure
and the lattice constants became smaller by
Co substitution. Taking the ionic radii of
Mg and Co into account, the results reﬂectthat Co occupies 4c (Ga, Mg) site. Rietveld
analysis using neutron diffraction patterns
indicated that both LSGM and LSGMC
could be attribute to orthorhombic Pnma at
298˜680 K. The oxygen content calculated
from the site occupancy decreased with increasing temperature in LSGMC while thatwas essentially independent of temperature in LSGM. These behaviors are consistent with results of oxygen nonstoichiometry measurements. Based on the reﬁned
structure, we estimated the nuclear densities with MEM. As a result, it was indicated that the oxygen nuclear density began to spread as temperature increased andthat such a tendency was more signiﬁcantin LSGMC than LSGM. This may correspond with higher conductivity of LSGMC
than LSGM. From the difference between
the nuclear densities at 298 K and 680 K
in LSGMC, it was suggested that oxygen at
O1 site diffused toward the neighboring O2site and vice versa.

From XRD patterns, it was consideredthat both LSGM and LSGMC had a sinActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-1-20
Structural evaluation of nanotube and nanosheet layered titanate with novel
nanostructures by neutron diﬀraction method
Takashi Kubo*, Masatomo Yashima, Atsushi Nakahira**Department of Materials Science, Graduate School of Engineering, Osaka Prefecture
University, 1-1 Gakuen-cho, Naka-ku, Sakai-shi, Osaka, 599-8531, Japan, Department ofMaterials Science and Engineering, Interdisciplinary Graduate School of Science andEngineering, Tokyo Institute of Technology, Nagatsuta-cho 4259, Midori-ku, Yokohama,226-8502, Japan
Currently, the development of synthetic
processing for various nanoscale materials is under intensive investigation1-3. Especially, titanate or titanium oxide based
nanotubes, which are prepared by a soft
chemical hydrothermal treatment of TiO2
particles in a highly concentrated NaOH
aqueous solution, received much attention, because they are expected to be useful for various applications such as photocatalysts and solar cells etc form theirnanotubular structures and high surface
areas4,5. Furthermore, these TiO2-derived
nanotubes synthesized by a soft chemical hydrothermal treatment possess ion exchange ability, such as sodium or hydrogen and have unique layered structures6-8.
However, the clariﬁcation of detailed structure of nanotubes is still insufﬁcient forthese TiO2-derived nanotubes synthesized
by a soft chemical hydrothermal treatmentby the conventional analysis technique.
Especially, since these TiO2-derived nanotubes synthesized by a soft chemical hydrothermal treatment of TiO2 contain hydrogen in its nanotubular structure, theneutron powder diffraction analysis is useful for clariﬁng these nanotubular titanate.
In this study, the fabrication of the titanate
nanotubes have been attempted by a soft
chemical hydrothermal treatment of TiO2
with a NaOH aqueous solution by the useof deuterated 10 M NaOH solution duringa soft chemical hydrothermal treatment of
TiO2.
Nanotubular titanate products weresynthesized by the soft chemical processing, that is, hydrothermal treatment in
NaOH solution and subsequently the eval-uation of its structure was attempted by
the neutron diffraction method. The detailed experimental procedures are described elsewhere6-8. Products were synthesized in deuterated 10 M NaOH solution at 383 K for 96 hours by the hydrothermal treatment. Products were ﬁltered with Buchner and washed sufﬁciently with deuterated water. Samples
were dried and crashed with Al2O3 mortar.
The neutron powder diffraction experiments were conducted using the neutron
powder diffractometer installed on Tl-3
port of JRR-3M reactor in the Japan Atomic
Energy Research Institute (JAERI), Tokai,
Japan. Neutron powder diffraction experiments were carried out in air at room
temperature. Neutron powder diffraction
measurements were conducted in air atmosphere with a 150-detector system, HERMES. An incident neutron wavelength λ =0.18196 nm was obtained from a Ge (311)monochromator. The ND data were collected on thoroughly ground powders by amultiscanning mode in the 2 θ range from5°to 155°with a step width of 0.10°. The 3 g
powder sample was wrapped by tungsten
foil to form a cylindric shape (10 φ× 30mm). The characterization of as-preparedtitanate products in deuterated NaOH solution by hydrothermal treatment and subsequently washed with deuterated water
was evaluated.
These products possessed nanotubular nanostructure with a few nanometerin diameter and some hundred nm inlength and identiﬁed to be H2TinO2n+1
as shown in Figure 1(A). From TEM ob-

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

servation (not shown here), these products
were open-ended nanotubes with average
inner diameter of approximately 5 nm andouter diameter of approximately 10 to 15
nm. The products had high surface areover 200 m2/g. Figure 1(B) shows the results of neutron powder diffraction for asprepared titanate products in deuterated
NaOH solution by hydrothermal treatment. In this study, some sharp peaks wereconﬁrmed by the neutron powder diffraction measurements. From the neutron powder diffraction measurements, the background of the neutron powder diffraction
pattern was high. This is caused by the insufﬁcient exchange of hydrogen and deuterium. These results suggest that TiO2derived nanotubes synthesized by a soft
chemical hydrothermal treatment at 383 K
contained some anatase structures. Thus,
the further study on the effect of synthetic
condition on the structure of nanotube titanate derived from TiO2 is needed for the
precise investigation.
1. S. Iijima, Nature, 354, 56 (1991).
2. P. Hoyer, Langmuir, 12, 1411 (1996)
3. T. Kasuga, M. Hiramatsu, A. Hosono, T.
Sekino and Niihara, Langumuir, 14, 3160
(1998).
4. G. H. Du, Q. Chen, R. C. Che, Z. Y. Yuan
and L. M. Peng, Appl. Phys. Lett., 79, 3702
(2001).
5. Q. Chen, W. Zhou, G. Du and L. M. Peng,
Adv. Mater, 14, 1208 (2002).
6. A. Nakahira, W. Kato, M. Tamai, T. Isshiki, K.Nishio and H. Aritani, J. Mater.
Sci., 39, 4239 (2004).
7. A. Nakahira, T. Kubo, Y. Yamasaki, T.
Suzuki and Y. Ikuhara, Jpn. J. Appl. Phys.,44, 690 (2005).
8. T. Kubo, W. Kato, Y. Yamasaki and A.
Nakahira, Key Eng. Mater., 317-318, 247(2006).

Fig. 1. Figure 1 (A) conventional XRD and (B) neutron diffraction result

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JAEA-Review 2011-050

1-1-21

Neutron Critical Diﬀuse Scattering of Quantum Relaxor KTaO3:Li
Hiroko Yokota and Yoshiaki Uesu
Deaprtment of Physics
Because the phase transition temperatureof KLT-6.8% is 87 K, the distribution of the
diffuse scattering is measured at 90 K. It
is known in relaxors that polar nano regions (PNRs) starts to appear at the Burns
temperature Td which is higher than the
dielectric maximum temperature. Therefore, measurements to observe diffuse scatterings from PNRs should be performed
above the phase transition temperature. In
the diffuse scattering distributions around(110) at room temperature and 90K, a streak
elongating along the [100] direction is observed at both temperatures. The origin is
not clear at present. However it exists evenat room temperature, therefore the existence is not related to the change in thepolar state in KLT. So we neglect the effect when we analyze the diffuse scattering due to PNRs. At 90 K, the intensity
along [-1 1 0] direction becomes stronger,
which signiﬁes the occurrence of the mosicity. It is observed that the tail of the diffuse
scattering intensity expands along the [100]and [010] directions to form a crossed rod.
The diffuse scattering from PNRs does notappear at the (220) reciprocal point. Thisphenomenon is coincident with the resultof Toulouse et al. The temperature dependence of the diffuse scattering at (1.032, 1,0) reciprocal point shows that below 80 K,
the diffuse scattering intensity begins to increase with decreasing temperature probably because of the inﬂuence of Bragg intensity. With heating the specimen, the diffuse
scattering increases abruptly and shows apeak around 85 K, which indicates the ﬁrst
order nature of the ferroelectric phase transition at Tp. the q dependence of the diffuse scattering is shown. Although a clear
disappearance of the diffuse scattering intensity which is expected at Td is not observed, the intensity decreases toward 160
K. This fact does not contradict our conclu-

sion that Td is located around 140 K by our
X-ray diffraction measurement.

Fig. 1. 逆格子点 (1 1 0) 周辺における散漫散乱測定

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1-1-22
Dependence of crystal structure and ferroelectric property on composition andheat treatment for (Pb,Si)(Zr,Ti,Nb)O3 ferroelectric material
Yasushi Idemoto and Shoko Komiya
Department of Pure and Applied Chemistry, Faculty of Scince and Technology, Tokyo
University of Science, 2641 Yamazaki, Noda-shi, Chiba 278-8510
In Ferroelectric random access memory(FeRAM), PbZrzTi1-zO3 (PZT), which isone of the most widely study ferroelectricmaterials, is considered as a candidacy
because of high remanent polarization(Pr). However, poor ferroelectric reliabilityof the PZT capacitor is a long-standing
problem, and there are many studies on
improvement of the electrode material.
For improvement of these problems,
we have synthesized the bulk samplesof(Pb0.98Si0.02)(ZrzTi0.95-zNb0.05)O3,(z=0.2˜0.5) and (Pb1-ySiy)(Zr0.30Ti0.7xNbx)O3, (x=0˜0.10; y=0.02, 0.04) [PZTNS]
ferroelectric materials prepared by asolid-state reaction. We investigated therelationship between the properties, crystal
structure and ferroelectric characteristics.
Nb was substituted up to 0.05 in thesamples by adding PbSiO3 (PSO).
As for the products, we characterized
their phases by XRD, compositions by Inductively Coupled Plasma(ICP) and EDX.
P-E hysterisis loop was measured at room
temperature by TF-2000. Capacitance andtan δ was measured by using LCR meter. We measured powder neutron diffraction using HERMES of IMR at the JRR-3M,
and determined the average crystal structures using the Rietveld method on thebasis of space P4mm with Rietan-2000[1].
These measurements were performed at
298K. The nuclear densities were also estimated based on MEM using the PRIMA[2].

shape, and the remanent polarization (Pr)increased and the coercive ﬁeld (Ec) decreased with Nb substitution. Moreover, Pr
increased and Ec decreased with the increasing PSO addition content. From thecrystal structure analysis, the position of
the M(Zr, Ti, Nb) site moved to the ideal
position with the Nb substitution. The formation of the oxygen vacancies was suppressed since the bond valence sum of theM(Zr, Ti, Nb)O6 octahedron increased. The
ﬂatness of the M(Zr, Ti, Nb)-O2 plane increased by the Nb substitution[3]. It is suggested that these factors lead to the squareness of the hystersis loop and improves theferroelectric property.
References[1] F. Izumi and T. Ikeda, Mater. Sci. Forum,
198,321(2000).
[2] F. Izumi and R. A. Dilanian, ”Recent
Research Developments in Physics,” Vol.
3, Part II, Transworld Research Network,
Trivandrum (2002), pp.699-726.
[3] Y. Idemoto, S. Komiya, Mater. Tech., inprint.

The lattice parameter ratio, a/c ,of PZTNS samples decreased compared to
PZT. The relative densities of pellets were
almost over 95%. From the P-E hysteresis measurements, the hystersis loop of the
Nb substituted PZTNS has a good square
Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-1-23Structural Defect and Ionic Conduction of Hydroxyapatite
H. Fujimori(A), K. Okanishi(A), K. Ohoyama(B), M. Yashima(C)(A)Graduate School of Science and Engineering, Yamaguchi Univ, (B)Institute for Materials
Research, Tohoku Univ., (C)Interdisciplinary Graduate School of Science and Engineering,Tokyo Institute of Technology
Hydroxyapatite is one of the most interesting materials in current technologies
due to its wide possible applications as biomaterials and electrical devices. Its physical and chemical properties relating to suchuses strongly depend on the crystal structure. Especially the stability of OH ion in
the structure of hydroxyapatite has beensuggested to be closely related to decomposition and ionic conductivity of hydroxyapatite. The OH lattice sites have been reported to be the conduction path of hydroxyapatite and to play an important role in
the proton conduction. Thus, it is of vital
importance to study OH ion at wide region of temperatures. However, information of hydrogen and oxygen ions is difﬁcult to be detected by the powder X-ray
diffraction (XRD) technique. The information contained in the characteristic spectral features of the OH group leads to theidentiﬁcation of important structural characteristics that cannot be made by XRD.
Previously we performed Raman scattering of hydroxyapatite at temperatures up
to 1200 oC by a new system of ultraviolet (UV) Raman spectroscopy. However,this technique is physically impossible todecide the position and diffusion path of
proton. Thus, in this study we have successfully determined the position and diffusion path of deuterium in hydroxyapatiteusing neutron powder diffraction data by
a whole-pattern ﬁtting approach based on
the maximum-entropy method (MEM).
Neutron powder diffraction dataof deuterium-substituted hydroxyapatitewere collected at 23 K, 300K, 673K, and1073 K using the HERMES powder diffractometer installed at the JRR-3M research reactor of the Japan Atomic Energy Agency.
Incident neutrons with a ﬁxed wavelengthof 1.8265(1) angstroms were obtained bya vertically focusing (331) Ge monochromator. The powder diffraction data were
measured over a 2 theta range of 6-156 degrees. The diffraction data were analyzed
by a combination of the Rietveld method
and MEM using the computer programs
RIETAN-FP and PRIMA. The space group
was assumed to be P21/b for the structure
at 23 K and 300 K. The reﬁnements of thestructure at 673 K and 1073 K were undertaken in P63/m. MEM analysis was conducted with the structure factors obtained
from Rietveld analysis.
The ﬁgure 1 shows the scattering amplitude distribution of hydroxyapatite with
P63/m structure at 1073 K, indicating deuterium ionic conduction along [001] direction. On the other hand, deuterium ion wasalmost localized at 673K, where the conductivity has been reported to be low.

Fig. 1. The scattering amplitude distribution of hydroxyapatite with P63/m structure at 1073 K drawn
by VESTA.

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JAEA-Review 2011-050

1-1-24

Neutron diﬀraction study on SnO2-CeO2 system
K. Nomura (A), H. Kageyama (A), T. Maekawa (B), C. Minagoshi (B), S. Nakamura (B),and T. Ito (B)(A) National Institute of Advanced Industrial Science and Technology (AIST), (B) New Cosmos
Electric Co., Ltd.
Recently, SnO2-based materials have been
investigated as transparent conductive oxides, oxidation catalysts, and the sensing
materials of semiconductor gas sensors [1].
Of these, as the sensing materials of sensors, SnO2-MOx (M = Al, Ce, etc.) systems have been mainly used. However,the detailed crystal structures of these systems are not clear yet. In the present study,
we measured the neutron diffraction dataof SnO2-CeO2 system at room temperature(297K), and investigated the crystal structure and the nuclear density distributions.
High purity (SnO2)(CeO2)x powder samples were prepared by a solid-state reaction method. Neutron diffraction measurements were performed with HERMES installed at JRR-3M in JAEA (Tokai) [2]. Neutron wavelength was 1.8265(1)A. Diffraction data were collected in the 2 θ range
from 20 to 153 deg in the step interval of
0.1 deg. The diffraction data obtained wereanalyzed by the combination technique of
Rietveld analysis using a computer program RIETAN-2000 [3] and a maximumentropy method (MEM)-based pattern ﬁtting. MEM calculation was carried out using a computer program PRIMA [4].
All the reﬂection peaks of (SnO2)(CeO2)x(x = 0, 0.03) were indexed by a tetragonal symmetry (P42/mnm, No.136). The
assumed structure model was as follows:
Sn4+ and Ce4+ ions occupy 2a sites (0, 0,0) and oxide-ions occupy 4f sites (x, y, 0) (x= y ˜ 0.36) [1]. The lattice parameters (a,c) and unit cell volume (V) increased withan increase in CeO2 content, suggesting an
introduction of larger Ce4+ ions (0.97A)[5] into Sn4+ (0.64A) [5] sites. The pureSnO2 sample showed narrow peak widthand low background intensities, whereas
the CeO2-doped samples wide peak widthand higher background intensities.
Figure 1 shows (a) the crystal structure and (b) the equicontour surfacesof scattering amplitude (0.05fm/Aˆ3) of(SnO2)(CeO2)0.03. The nonsphere-shaped
equicontour surfaces appeared at 4f (oxideion) sites.
References[1] M. Batzill and U. Diebold, Progress in
Surface Science, 79, 47 (2005).
[2] K. Ohoyama, T. Kanouchi, K. Nemoto,
M. Ohashi, T. Kajitani, and Y. Yamaguchi,
Jpn. J. Appl. Phys., 37, 3319 (1998).
[3] F. Izumi and T. Ikeda, Mater. Sci. Forum,
321-324, 198 (2000).
[4] F. Izumi and R.A. Dilanian, in: Recent
Research Developments in Physics, vol.3,
Transworld Research Network, Trivandrum, 2002, p.699.
[5] R.D. Shannon, Acta Cryst., A32, 751(1976).

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

Fig. 1. (a) Crystal structure and (b) equicontour
surfaces of scattering amplitude (0.05fm/Aˆ3) of(SnO2)(CeO2)0.03.

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JAEA-Review 2011-050

1-1-25Magnetic Phase Transition and Electric Polarization Flop of TmMn2 O5
M. Fukunaga1 , K. Nishihata1 , H. Kimura1 , Y. Noda1 , and K. Kohn2
1 IMRAM, Tohoku University, 2 Waseda University
bly for the ﬁrst time. The inset shows theobserved D–E hysteresis loop along the aaxis at 4.3 K, in which the linear permittivity component is subtracted.
The two magnetic phases exhibit almost
the same magnetic propagation wave vector, but different magnetic structures cause
the different dielectric properties. Magnetic structure analyses of both phases are
required to discuss the difference between
the two phases.
(a)

qx

0.47

0.46

(b)

qz

0.29

Integrated intensity

0.28
LT-ICM2 / LT-ICM1

(c)

/
/

E // b
E // a

0.5

0.0

-2

1.0

0.0
2.5

0.3

D /nC·cm-2(d)
Pr /nC·cm

We have performed simultaneous measurements of magnetic neutron diffraction,
ferroelectric D–E hysteresis loops and thepermittivity along the a-axis of TmMn2 O5
at FONDER. TmMn2 O5 is a rare-earth (R)manganese oxide of the form RMn2 O5 ,which is known as multiferroic materials
that exhibit coupling between ferroelectricity and magnetic ordering. It is believed that ferroelectricity of RMn2 O5 appears only along the b-axis, and application of the electric ﬁeld along the a-axis has
not been performed. It was observed thatneither the neutron diffraction proﬁles nor
the phase transition temperatures dependon the applied electric ﬁeld along the a-axis
as well as the b-axis. But interesting results
were obtained by the simultaneous measurement.
Figure 1 exhibits simultaneous measurement results of the magnetic propagation
wave vector q x , qz , integrated intensity,and the remanent polarization along aand b-axes of TmMn2 O5 below 6 K, wherea low-temperature incommensurate magnetic phase (LT-ICM1) changes into anothermagnetic phase (LT-ICM2). The ﬁlled symbols (with the electric ﬁeld along the aaxis), the open symbols (b-axis) and q x were
measured separately. Although the dielectric properties along a- and b-axes of thesame sample cannot be measured simultaneously, neutron diffraction results measured simultaneously with the dielectric
properties guarantee the temperature axisof the two experiments. It was clearly obserbed that the decrease in the polarization
along the b-axis coincides the decrease in
the LT-ICM1 phase, and the increase in thepolarization along the a-axis coincides theincrease in the LT-ICM2 phase. As a result,it seems that the polarization ﬂops from theb-axis to the a-axis. The polarization along
the a-axis of RMn2 O5 was observed proba-

Pb

0.0

-0.3
-5

3.0

0

E /kV·cm

-1

3.5

4.0

5

Pa

4.5

5.0

5.5

6.0

Temperature /K

Fig. 1. Simultaneous measurement results of (a) the
propagation wave vector q x , (b) qz ,(c) integrated intensity, and (d) remanent polarization along a- andb-axes, Pa and Pb of TmMn2 O5 during cooling.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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1-1-26

Split-hydrogen sites in trioctahedral micas
Kiyotaka Ishida and Hiroshi Fukazawa
Kyushu University, Japan Atomic Energy Agency
Two
kinds
of
the
deuterated
tetra-germanium
magnesium
micas,
KMg2.5Ge4O10(OD)2and
KMg2.5(Ge3D4)O10(OD)2,
have
synthesized by a Tuttle type cold-sealdhydrothermal equipment, and their neutron diffraction data were obtained insuccess by HERMES. Their crystal structure reﬁnment have done by Rietan-2000.
Further sructure analysis are on the move.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-1-27
Powder Neutron Diﬀraction Measurements of One-dimensional Magnets
MPb4 Sb6 S14 (M = Fe, Mn)
Yoshitaka Matsushita1 , Masakazu Nishi2 , and Satoshi Watanabe2
1 Quantum Beam Center, National Institute for Materials Science
2 Institute for Solid State Physics (ISSP), The University of Tokyo
One-dimensional (1D) Heisenberg antiferromagnetic chain (HAF) compounds
in magneto-chemistry and physics ﬁelds
have attracted considerable interest, because most of them have been served asa prototypical model in quantum statics.
Haldane theoretically predicted that 1DHAF systems having integer spin quantum number (S = 1, 2, · · ·) should have aspin energy gap called as Haldane-gap between the ground state and the ﬁrst excitedstate, in contrast to the case of half-integer
spin quantum number (S = 1/2, 3/2,
· · ·). [1] Since Haldane s prediction, extensive studies have been carried out on
1D-HAF systems with integer S. In 1986,
the ﬁrst S = 1 compound with Haldane
gap, [Ni2+ (en)2 NO2 ](ClO4 ) (so called as
NENP) was discovered by Renard and his
co-workers as the real system. [2] After the
discovery of this compound, some of S = 1
Haldane gap compounds have been studied. [3]We propose the rare S = 2 Haldane candidate mineral semiconductor compound,Fe2+ Pb24+ Sb36+ S214− (Jamesonite, hereafterFPSS). It is the isomorphic compoundof Mn2+ Pb24+ Sb36+ S214− (Bénavidésite, hereafter MPSS). The several properties (structural, thermal, optical, electrical, magnetic
properties) and synthetic condition of thesecompounds, had been reported. [4, 5, 6, 7]
The monoclinic crystal structures of FPSS
and MPSS consist of the lozenge-shaped[Pb4 Sb6 S13 ] and the rod-shaped [MS6 ] substructures (Fig. 1). In the structure, Fe2+
(d6 ; S = 2) is located at the origin site
(Wyckoff position; 2a in P21 /a) and octahedrally coordinated by six sulfur atoms.
The [FeS6 ] octahedra form the edge-shared
1D linear chain, running along the c-axis,

as shown in Fig. 1. The shortest Fe· · ·Fe
distance is 4.030(4) Å within the chain and12.388(6) Å between the chains. Therefore, the magnetic inter-chain interaction
should be weak, and FPSS can be regarded
as an ideal 1D magnetic chain system with
S = 2. From these crystallographic andmagnetic properties, FPSS is expected to
be a candidate of S = 2 Haldane compound. Apart from the argument of S =2 Haldane compound, S = 2 1D magnetic chain compound itself is rare. In
the magnetic susceptibility measurements,
FPSS showed 1D HAF behavior with abroad peak around 33.5 K, where a highspin state (S = 2) of Fe2+ was estimatedfrom a Curie-Weiss law ﬁtting of magnetic
susceptibility. Under 10K, FPSS shows two
anomalies at ∼ 8 K and ∼ 3 K. [4, 5, 6]
On the other hand, MPSS shows a broad
peak around 25 K, and in lower temperature range small Curie tail are observed.
However, both FPSS and MPSS did notshow any long range ordering behaviors
from results of magnetic susceptibilities(AC and DC), heat capacity and Mössbauer
measurements, both compounds showedspin-glass behavior under low temperature
range. [5, 6, 7] In 2004, Léone et al. reported
powder neutron measurement using natural FPSS, and they observed extra peaks
to be caused by magnetic long-range ordering. [8] The result is not consistent with
our results. In this study, we carried out
neutron powder-diffraction measurements
using synthesized FPSS and MPSS compounds to understand magnetic behaviors
these compounds.
The samples were prepared by solidstate reaction. [5] The neutron powderdiffraction measurement (7◦ ≤ 2θ < 157◦ )Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

was carried out using IMR-HERMES diffactmetor (T1-3), installed in the JRR-3M
reactor. The wavelength of neutron was
1.8265(1) Å, which was vertically focusedby a (331) Ge monochromator. The intensity data was observed at 4.0 K for FPSS
and 1.4 K for MPSS, respectively.
Around 15.5◦ in 2θ, weak peaks areobserved, but they are not matchedwith Léone’s proposed magnetic orderingmodel. [8] To understand the details ofmagnetic behaviors of the compounds weneed to examine under lower temperature
with the higher resolution facilities.
References[1] F. D.M. Haldane, Phys. Rev. Lett. 50 (1983)
1153.
[2] J. P. Renard et al., Europhys. Lett. 3 (1987)
945.
[3] K. Katsumata, Current Opinion Solid State
Mat. Sci. 2 (1997) 226, and references
within.
[4] P. Léone et al., Solid State Sci. 5 (2003) 771.
[5] Y. Matsushita, Y. Ueda, Inorg. Chem. 42(2003) 7830.
[6] Y. Matsushita, Y. Ueda, Prog. Theor. Phys.
159 (2005) 179.
[7] S. Morimoto et al., J. Mag. Mag. Materials
310 (2007) e962.
[8] P. Léone et al., J. Mag. Mag. Materials 284(2004) 92.

Fig. 1. 1) 1D-chain structure in FPSS. 2) Magnetic susceptibility of FPSS. 3) Neutron powderdiffraction diagram.

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JAEA-Review 2011-050

1-1-28

Crystal Structure of La-Ge-O Ionic Conductor
Yoshitaka Matsushita, Naohito Tsujii, Kiyoshi Kobayashi, and Fujio Izumi
Quantum Beam Center, National Institute for Materials Science
was selected to P1̄, and both reported structural models were examined. In current
reﬁnement process, the Pramana’s modelgave better ﬁt. However, the reﬁnement
is not fully satisﬁed. The current convergent indexes were Rwp = 3.96 %, Rp = 2.93%, RR = 6.15 %, Re = 0.78 %, RI = 0.89 %,and RF = 0.41 %. The obtained cell parameters from the Rietveld analysis were a =9.929(2) Å, b = 9.920(2) Å, c = 7.2914(6) Å, α= 90.46(1) ◦ , β = 89.04(1) ◦ , and γ = 120.36(1)◦.
References[1] S. Nakayama et al.: J. Mater. Chem. 5 (1995)
1801.
[2] S. Nakayama et al.: Chem. Lett. 24 (1995)
431.
[3] L. Leon-Reina et al.: Chem. Mater. 15 (2003)
2099.
[4] S. P. Pramana et al.: Acta Crystal. B63 (2007)
597.
[5] F. Izumi and T. Ikeda: Mater. Sci. Forum
321-324 (2000) 198.
[6] F. Izumi and R. A. Dilanian: Recent Res.
Develop. Phys. 3 (2002) 699.
70000
60000

Intensity (counts)

The La-T (T = Si and Ge) oxyapatites
having chemical composition written as
Ln9.33 ± x T6 O26 ± 3x/2 , attract attention forthe most promising oxygen-ionic conductor of next generation, and it has beenmeasured the various kind of properties
until now.[1, 2] These compounds show
better oxygen ionic conductivity in theintermediate-temperature range comparedwith other famous oxygen-ionic conductors (ZrO2 and/or CeO2 -based materials). However, the excess oxygen sites
have not been found out, yet. The germanate compounds have low-temperature(P1̄) and high-temperature (P63 /m) forms.
The two crystal structure models of lowtemperature form had been proposed.[3,4] In this study, we measured the intensity data using neutron powder-diffraction
technique to identify the crystal structureof low-temperature germanate.
The
germanateapatitesample(La9.8 Ge6 O26.7 ) was prepared by solidstate reaction. All processes are carriedout under air. The mixture of La2 O3 andGeO2 were calcined at 1273 K for 50 hours.
Starting La2 O3 was pre-heated at 1273
K for a night. The ground sample waspressed into the pellets, and re-heated up
to 1273 K for 24 hours.
The intensity measurement at room temperature (5◦ ≤ 2θ < 156◦ ), was carriedout using IMR-HERMES diffactmetor (T13), installed in the JRR-3M reactor. The
wavelength of neutron was 1.8265(1) Å,
which was vertically focused by a (331) Ge
monochromator. The resulting diffraction
data were analyzed by the Rietveld methodwith RIETAN-FP [5] and whole-pattern ﬁtting approach based on the maximumentropy method (MPF)[6].
The cation compositions were ﬁxed as
chemical analysis result (La9.8 Ge6 O26.7 ) on
the Rietveld reﬁnement. The space group

50000
40000
30000
20000
10000
0
10

20

30

40

50

60

70

80

2q (°)

90

100

110

120

130

140

150

Fig. 1.
Powder neutron diffraction proﬁle of
La9.8 Ge6 O26.7 .

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 500

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JAEA-Review 2011-050

1-1-29Low energy excitation in DyB6
K. Tomiyasu and K. Takahashi
WPI-AFIR Tohoku University and IMR Tohoku University
The freedoms of orbital and quadrupole
are established as real existence. However, the excited states (the orbital wave
and quadrupole wave) are not sufﬁciently
studied in the experiments. Only few materials were measured by Raman scattering. Therefore, we submitted the trial measurements of low energy phonon in DyB6
on HER (C1-1) in order to obtain the dispersivity of the quadrupole wave or thequadrupole-lattice coupling. DyB6 exhibits
the quite high transition temperature offerro-type quadrupole ordering TQ =32 K( 3 meV), and the Q value and the temperature region of the ordering are distinguished from the antiferromagnetic order(TN =23 K). The effect of quadrupole orderon phonon can be extracted under 3 meV
between TQ and TN .
The experimental conditions are summarized as follow: G-M-O-PGF-S-80’-BeFﬂatA-80’-C, E f =6 meV, narrowers (8×20mm2 , 21×40 mm2 ), GM-CTI, 1 single crystal with mm edge, hhk zone, standard
Al-can. Figure 1(a) shows the constantQ scans at hh2 (h=0.02, 0.04, 0.06, 0.08) at
T=29 K (TN < T < TQ ). The Q positions
give us the TA phonon with the polarization along the [001] direction and the propagation vector along the [110] direction.
Only the data at 0.04 0.04 2 show the appreciable peak. Figure 1(b) shows the temperature dependence of constant-Q scans at
0.04 0.04 2. The spectrum lines are ﬁtted by
the two Gaussians of the incoherent elastic
scattering and the TA phonon. The ﬁtting
parameters are obtained to be E=1.02, 1.24
and 1.37 meV and ΔE(FWHM)=1.27, 1.47
and 0.95 meV at 29, 35 and 50 K, respectively. We now compare the neutron datawith the ultrasound data, and discuss thesoftening of the phonon in connection withthe spatial size of the quadrupole order domain, which is expected to be distributed

from micro-m to nano-m.

Fig. 1. (a) Constant-Q scans at T=29 K. (b) Temperature dependence of constant-Q scans at 0.04 0.04 2.

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1-1-30High resorution inelastic neutron scattering by TiNi(Fe) alloy
T. OHBA(A), D. KITANOSONO(A), T. FUKUDA(B)(A) Department of Materials Science, Shimane University, (B) Materials Science andEngineerng, Osaka University
TiNi alloy system exhibits martensitic
transformation, which shows typical ﬁrstorder transformation. A few percent Fe
added and substituted by Ni alloys were
utilized for fundamental studies of martensitic transformation about 20 years ago. Rphase was found through the research andwas thought at the beginning to be a precursor state of martensite. Later the Rphase was understood to be another typeof martensite, whose structure was determined by Hara et al. Recently, systematicstudies of Fe added alloys more than 2 percent were carried out. Calorimetric measurements and electrical resistivity measurements indicated different transformation behavior from ﬁrst-order transformation for six or eight atomic percent alloys;that is Ti50Ni44Fe6 or Ti50Ni42Fe8. Calorimetric measurements show no transformation peak for those alloys. Electron diffraction studies and X-ray diffraction studies
were also carried out for those alloys. Crystal structure of high temperature phase is
B2 (CsCl) type. Diffuse peaks appeared
around 1/3 of <110>* with lowering temperature. Those electron diffraction patterns were similar to diffraction patternsof R-phase. Since the martensitic transformation is known to be displacive transformation, phonon behavior is attractive
mechanism for understanding the transformation. From the structural knowledge, [zz0]TA2 mode was expected to besoft at the transformation temperature.
Ohba et al. measured phonon behavior
for TiNi system previously. However noclear phonon softening was observed. Inelastic scattering measurements for larger
than z=0.3, which is most important partof the phonon, showed disturbed peaks.
Therefore, precise and high-resolution experiments were required. Inelastic scatter-ing measurements for [zz0]TA2 mode werecarried out at various temperatures. Figure 1 showed neutron inelastic experimental data for the alloy measured at 180K.
Electron diffraction patterns at the temperature indicated R-phase like pattern. Incoherent intensities were subtracted from theobserved data and shown in the ﬁgure, simultaneously. Inelastic phonon peak wasfound close to E=0, which may indicate almost complete softening of martensitic materials.

Fig. 1. Inelastic scattering data for [zz0]TA mode at
180K. The row data and incoherent intensities subtracted data were plotted.

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1-1-31
Crystal Structure Analysis of a Supramolecular Ferroelectric 55DMBP-H2 ia
R. Kumai(A), D. Okuyama(B), S. Horiuchi(A), T. Arima(C), M. Watanabe(C), Y.
Noda(C), and Y. Tokura(A,B,D)(A)CERC AIST, (B)Multiferroic Project, ERATO, JST, (C)IMRAM, Tohoku Univ. (D)Dept.
Appl. Phys., Univ. Tokyo
Ferroelectrics have been motivated not
only by basic science but also by application because of those various utilizations for electronics. Recently Horiuchi etal. have reported a new ferroelectric realized by proton dynamics in a hydrogenbonded chain with supramolecular structure, the cocrystal of 5,5’-dimethyl-2,2’bipyridine (55DMBP, C12 H12 N2 ) and iodanilic acid (H2 ia, C6 H2 O4 I2 ).[1] The previous X-ray crystal structure analysis worksuggests that the proton transfer occurs at
Curie temperature (TC = 268 K on cooling)
and the corrective proton motion shouldbe playing an important role for the development of the ferroelectricity in this material. Here, we report the crystal structureof 55DMBP-H2 ia obtained by the neutron
diffraction in order to make clear the more
precise hydrogen atom position.
Large single crystals of 55DMBP-H2 ia(3 × 1 × 10 mm3 ) were prepared by slow
evaporation from methanol solution. Neutron diffraction experiments were performed by utilizing a four-circle diffractometer FONDER with 1.245 Å neutron beam monochromized by a Ge(311)monochromater. We used the program
DABEX for the absorption correction andthe calculation of the diffraction path
length which was used for extinction corrections. Using the corrected data sets, weused the program SHELX-97 for the leastsquare ﬁtting in order to reﬁne the parameters.[2]Figure 1a shows the crystal structure ofparaelectric phase of 55DMBP-H2 ia at T =300 K obtained by a neutron crystal structure analysis. Lattice parameters, spacegroup (P − 1), and atomic coordinates except for hydrogen atoms agree with thoseobtained by the X-ray diffraction exper-

iments. It can be clearly observed that
there are two types of hydrogen bondedsite in the crystal. The signiﬁcantly elongated thermal ellipsoid of hydrogen atomin the methyl group shows the rotational
disordering of the methyl group. One canﬁnd the slightly elongated thermal ellipsoid of one hydrogen nuclei (H2), whichindicates a broadly distributed hydrogenatom. From the interatomic distance table(inset of Fig. 1a), the migration of hydrogen atom of H2 site toward the center of the
N· · ·O hydrogen bond can be found. The
situation can be also observed in the nuclear density distribution obtained by the
maximum entropy method (MEM) analysis of the diffraction data. Figure 1b shows
the nuclear density distribution between
N· · ·O hydrogen bond. The broadly distributed nuclear density at H2 site indicatesthe proton disorder in the short N· · ·O
(2.58Å) hydrogen bonded site. In the lowtemperature phase, we can be observed
proton transfer at both H1 and H2 sites
from the X-ray structure analysis. Neutron
diffraction study of the ferroelectric phaseof the 55DMBP-H2 ia, which is planned innear future, can provide us for more precisely information of the proton dynamics
and the origin of polarization in the crystal.
References and notes [1] S. Horiuchi, R.
Kumai, Y. Tokura, Angew. Chem. Int. Ed.,46, 3497 (2007). [2] 55DMBP-H2 ia 300K:
C18 H14 N2 O4 I2 , Z = 2, Triclinic P − 1, a =10.14(3) Å, b = 8.81(5) Å, c = 12.782(15)Å, α = 67.05(7)◦ , β = 67.80(12)◦ , γ =67.06(10)◦ , V = 933(3) Å3 , R = 0.0343
for 1527 independent reﬂections (| Fo | >4σ (| Fo |)).

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Fig. 1. (a) Crystal Structure, (b) nuclear density distribution map, and nuclear densities of hydrogen
atom in the hydrogen bond for paraelectric phase(room temperature) obtained by the present neutron
diffraction study.

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1-1-32

Study suggests the existence of ferroelectric ice layer on a cold planet
Hiroshi Fukazawa, Hiroki Yamauchi, Akinori Hoshikawa
JAEA and Ibaraki Univ.
Whether ice in the outer solar system exists as hydrogen-ordered ices, is a questionthat has attracted scientiﬁc interest. Someordered ices have ferroelectricity, and longrange electrostatic forces caused by the ferroelectricity might be an important factor
for planet formation. Features of the infrared spectrum of proton-ordered structures are unknown because of the difﬁcultyin creating ordered ice in the laboratory.
The aligned water ices are obtained only by
doping of water samples with some catalysts, such as KOH or HCl, and the inﬂuence of the dopant on long-range ordering
was not well resolved.
We produced KOD-doped D2O powder with a homogeneous concentration of
KOD by rapid solidiﬁcation of a mist of
0.001 - 0.1 M KOD solutions. Diffraction
patterns were saved every 0.5 hours of collection time. These time-resolved measurements were performed at the HERMES in
04 and 05 [1, 2]. We have succeededin making large quantities of ferroelectricice, named ice XI, with the small amount of
KOD, and then maintaining the samples ina 50 to 75 K temperature range over several days. From proﬁle reﬁnements with
better values of reliability factors, which isthe best way of investigating deuteron ordering, we found the temperature condition for the transformation of the largest
fraction of ice Ih into ice XI. The ﬁnding
conﬁrms that ice XI is in a thermodynamically stable phase at low temperatures. We
did longer experiments of same ice samples using a powder diffractometer, named
the WAND, at the Oak Ridge National Laboratory, Based on the results, we proposethat ice XI exists in the Universe [3]. It was
picked out by US and Japanese press [4].
In spring and summer of 07 we usedthe HERMES again and ﬁrst measured insitu time-resolved neutron diffraction of ice

with 0.01 M KOD, which compressed atabout 0.02 GPa using a sapphire cell of alarge single crystal. We observed a transformation to the ferroelectric ice XI in a 60
to 75 K temperature range over tens hours.
The results show that the ferroelectric ice
is stable below 0.02 GPa. It suggests that athick layer of ferroelectric ice exists on thesurface of Pluto (Figure). Future telescopeor planetary probe will be able to detecte
the huge ferroelectric-ice mass.
We plan to do in-situ experiments
on ice under much higher pressure conditions up to 10 GPa in 08 . We try to observe the phase transition from disorderedphases to the ferroelectric ice or other ordered phases around 40-130 K (The value isthe same as the temperature of Pluto’s surface and inner). The experiment will reveal
the whole picture of low-temperature ice
structures. It will show that myriad big icybodies in outer solar system, which exist
as dwarf planets and KBO, consist of thickferroelectric-ice surface and several inner
layers of hydrogen ordered ices.
References[1] H. Fukazawa, A. Hoshikawa, H. Yamauchi, Y. Yamaguchi and Y. Ishii, J. Crystal Growth 282 p.251 (2005).
[2] H. Fukazawa, et al., Physica B 385-386
p.113 (2006).
[3] H. Fukazawa et al., Astrophysical Journal Letters 652, pp.L57 (2006).
Choice,2007,
Sci[4]
Editor s
ence
315,
18;
PhysOrg.com(http://physorg.com/news83862687.html);
inAsahi Daily Newspaper (2/2/07
Japanese); Tokyo Dainly Newspaper(7/10/07 in Japanese).

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1-1-33Structures and Phase Transitions in A2BO4-type Dielectrics
H. Shigematsu(A) and K. Nomura(A)(A)Department of Physics, Faculty of Education, Shimane University
Among a lot of A2BX4-type ferroelectrics(X = O, Cl, Br), a typical soft phonon-mode
was observed in K2SeO4 clearly both aboveand below the normal-incommensurate(N-INC) phase transition point by neutron
scattering. That is to say, the transitionin K2SeO4 is interpreted as a displacivetype one. On the other hand, since the softmode above the N-INC transition point
in Rb2ZnBr4, Rb2ZnCl4 and K2ZnCl4 was
not observed, it was thought that the transition type was an order-disorder one. For
many A2BO4-type crystals such as K2SO4,K2CrO4, Rb2SeO4 and Cs2SeO4, the NINC transition has never been reported.
However, in the case of K2CrO4 and
Rb2SeO4, the calculated dispersion curvescontain an unstable sigma2 phonon branchwhose qualitative and quantitative featuresare similar to those obtained for prototype incommensurate material K2SeO4. Indeed, a softening tendency of the sigma2
phonon branch around 0.7a* was observedin K2CrO4 and Rb2SeO4 [1]. The estimates
hypothetical temperature in Rb2SeO4 is below -150 K.
In order to clarify the mechanism of lowtemperature incommensurate phase transition and the hypothetical one in A2BO4type crystals, we have to obtain additional
information about the behavior of the lowenergy sigma2-sigma3 optical branches invarious A2BO4-type crystals. Therefore,
we performed inelastic neutron scattering experiments by use of the triple-axis
spectrometers (4G and T1-1) at JRR-3M of
JAERI.
Figure 1 shows the phonon dispersion
curves in an extended-zone scheme alongthe (x 0 0) direction for K2Se0.5Cr0.5O4.
Two modes, which were anticrossed toeach other around x ˜ 0.7, were observed.
It is clear that low-frequency mode softens slightly in the vicinity of x = 1 withdecreasing temperature, although the frequency will remain ﬁnite at 0 K. The estimated hypothetical temperature is about 160 K, which is lower than the calculated
hypothetical temperature.
In Cs2SeO4, whose calculated hypothetical transition temperature was -151 K,
the phonon dispersion frequency was essentially unchanged below room temperature. Our experimental results show thatthe plausible hypothetical temperature will
be lower. The inelastic neutron scattering
study on Rb2MoO4 is now in progress, because we found a new N-INC transition at
223 K.
References[1] H. Shigematsu et al., J. Korean Phys.
Soc. 46 (2005) 235.

Fig. 1. Phonon dispersion curves in an extendedzone scheme on the (x 0 0) for K2Se0.5Cr0.5O4.

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1-1-34Magnetic structure of Ni-Mn-Z(Z=In, Sn) shape memory alloys
T. Kanomata, K. Fukushima, Y. Yamaguchi(A)Faculty of Engineering, Tohoku Gakuin University, Institute for Materials Research, Tohoku
University(A)The Heusler alloys Ni2Mn1+xSn1-x(Z=In,
Sn and Sb) show the martensitic transition
from the L21 structure to an orthorhombic
four-layered one. Unlike the case of conventional ferromagnetic shape memory alloys, the magnetization in the martensite
phase for Ni2Mn1+xZ1-x(Z=In, Sn amd Sb)
is much smaller compared to that in theaustenite one. More recently, the present
author s group has found an magneticﬁeld-induced martensitic transition froma nonmagnetic martensite phase to a ferromagnetic austenite one in the Ni-MnSn Heusler alloy system. This alloy system opens up to the possibility of utilizing the magnetic-induced shape memory
effect. Since then, the magnetic shape memory alloys Ni-Mn-Z(Z=In, Sn and Sb) haveattracted much attention from the point ofview of high performance materials being
controlled by a magnetic ﬁeld.
To investigate the magnetic structure of thenonmagnetic martensite phase in Ni-MnSn magnetic shape memory alloys, we carried out the neutron powder diffraction experiments for Ni2Mn1+xSn1-x(x=0.44, 0.48
and 0.52 ).
The neutron powder diffraction pattern of Fig. 1(a) obtained at 370 K for
Ni2Mn1.48Sn0.52, up the Curie temperature(TC= 313 K), shows strong Bragg reﬂections all of which could be indexed on
the L21 fcc structure. The neutron powder diffraction pattern of Ni2Mn1.48Sn0.52
measured at 70 K, below the martensitic
transition temperature (TM= 300 K), isshown in Fig. 1(b). It contains no residual
cubic component. Most of the main reﬂections can be indexed using the 4O structure(space group: Pmma). It should be notedthat no satellite reﬂections are observed.
The analysis of the neutron powder diffraction is in progress to determine the mag-netic structure of Ni2Mn1+xSn1-x(x= 0.44,
0.48 and 0.52 ) in the martensite phase.

Fig. 1. Fig. 1 the neutron powder diffraction patterns of Ni2Mn1.48Sn0.52 at 370 K(a) and 70(b).

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1-1-35

Crystal Structure Determination of Ba2MgSiO7 by Neutron Diﬀraction
Satomi Seki, Akira Komeno, Kazuyoshi Uematsu, Kenji Toda, Mineo Sato
Niigata University
The emission depends on the environment of the emission ion site in the hostlattice. The silicate phosphors have relatively strong and rigid characteristics ofpartly covalent Si-O bond. In addition,
rigid frameworks often provide relatively
distorted coordination around the emission
ion. Therefore, strong crystal ﬁelds wereobserved in many silicate phosphors. Alkaline earth silicate phosphor, M2MgSi2O7(M = Ca, Sr and Ba) are expected as highluminance phosphor. However, the crystal
structure of Ba2MgSi2O7 has not been reported up to now. The powder XRD patternof Ba2MgSi2O7 differs from that of single
crystal Ba2MgSi2O7. In this study, we show
the crystallographic date on Ba2MgSi2O7
reﬁned from the neutron powder diffraction patterns.
Crystal structures of Ba2MgSi2O7, wereﬁrst reported by M. Shimizu et al. [1].
They reﬁned Ba2MgSi2O7 on the basis ofa tetragonal system with space group P421m (a = 0.8425 nm). The crystal structureof Ba2MgSi2O7 differs from the tetragonal
symmetry. Indexing of the XRD pattern forthe powder sample, Ba2MgSi2O7 has monoclinic system with space group C2/c (a= 0.8426 nm). However, since these structures were deduced only from the electron and powder X-ray diffractions, the information on light elements, especially foroxygen atom, was quite poor.
Figure 1 and Table 1 shows the powder neutron diffraction pattern ﬁtting andstructural parameters for the Ba2MgSi2O7.
All of the diffraction peaks were well indexed on monoclinic system C2/c. A goodﬁtting proﬁle were obtained with Rwp =5.65 %.
Tetragonal and monoclinic structures takesimilarly layered structures with different
barium coordination environments. It isconsidered that the synthesis temperature

and annealing time are most important factors whether Ba2MgSi2O7 take the twotype structure, tetragonal or monoclinic.
[1] Y. Lin, C. W. Nan, X. Zhou, J. Wu, H.
Wang, D. Chen, S. Xu. Mater. Chem. Phys.,
82 (2003) 860-863.

Fig. 1.

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1-1-36Diﬀuse Scattering Measurement on Protonic Conductor K3 H(SeO4 )2
F. Shikanai, S. Itoh, K. Tomiyasu A , N. AsoB , S. Ikeda and T. Kamiyama
Institute of Materials Structure Science, High Energy Accelerator Research Organization
A Institute for Materials Research, Tohoku University
B Institute for Solid State Physics, University of Tokyo
Much attention has been paid to somehydrogen bonded dielectric materials as
the electrolytes for fuel cells which function above the boiling temperature of water. K3 H(SeO4 )2 undergoes 1st order phasetransition at 390 K (TC ). The materialshows remarkable high electric conductivities above TC (Phase I) and ferroelastic below TC (Phase II). From the structural analyses by means of neutron diffraction, it developed that the slight deform of potassium lattice determine the hydrogen bonds
orientation in the phase II, and alternate rotational displacements of SeO4 tetrahedra
which explained as zone boundary phononmode correspond with the crystal structure in the phase II. [1, 2] We, therefore,
have carried out inelastic neutron scattering (INS) experiments to clarify the mechanism of protonic conductivities and ferroelastic phase transition. No soft mode wasobtained both of acoustic and zone boundary optical modes, however, diffusive spectra were obtained near the 0 meV at the Lpoint (0.5 2 0) above TC . The results suggestthat the rotational phonon mode of tetrahedra is to exist as over dumped phonon.
INS measurements were carried out using a high energy resolution triple axis
spectrometer (C1-1 HER) installed at JRR3M reactor, JAEA, Tokai, Japan. The energyscans were performed at zone boundary Lpoint with the energy transfer range from
-2 meV to 4 meV. Final momentum vector
kf was ﬁxed at 1.555 Å−1 . The h-scans from(0.25 2 0) to (0.75 2 0) were also performed
to conﬁrm that the INS spectra is obtainedat only L-point.
Figure 1 shows INS spectra measured
on the L-point by constant-Q mode atvaried temperatures near TC . Lorentzian
shape spectrum increases with decreasing

the temperature as shown in the ﬁgure.
The result is close to the spectra of overdumped phonon of CsPbCl3 due to the M3
mode tilts of PbCl4 octahedra. [3] It showsthat the rotational mode of SeO4 tetrahedra drives the improper ferroelastic phasetransition, and plays an important role tothe mechanism of proton conductivity inthe phase I. It naturally expected that tilted
tetrahedra form the hydrogen bonds locally even in the phase I, and the rotationalmode over-dumped by the formation ofhydrogen bonds. It developed that the hydrogen bonds disconnect and reconstruct
due to the rotational tetrahedra mode in
the phase I. It suggested that the rotationalmode assists in the protons jumping to theinter-layer space in the metastable state.
References[1] F. Shikanai et. al.: Physica B 385-386 (2006)
156.
[2] F. Shikanai et. al.: Ferroelectrics 347 (2007)
74.
[3] Y. Fujii et. al. : Phys. Rev. B 9(1974) 4549.

Fig. 1. INS spectra of K3 H(SeO4 )2 at L-point

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1-1-37Structural investigation of the cubic perovskite-type doped lanthanum cobaltite
La0.4Ba0.6CoO3-x
Takashi Ohta(A), Masatomo Yashima(A), Takahiro Wakita(A), Yoshitaka Matsushita(B),Takafumi Komatsu(A), and Yong Phat(A)(A)Department of Materials Science and Engineering, Interdisciplinary Graduate School of
Science and Engineering, Tokyo Institute of Technology, (B) Quantum Beam Center, National
Institute for Materials Science
Lanthanumstrontium
cobaltites,
La0.4Ba0.6CoO3-x,
which
have
a
perovskite-type structure, are promising electrode materials for the doped
lanthanum gallate electrolyte in solidoxide fuel cells (SOFCs). The purposeof the present study is to investigate
the crystal structure of the cubic Pm-3m
perovskite-type La0.4Ba0.6CoO3-x at room
temperature and at high temperatures.
La0.4Ba0.6CoO3-x pellets were supplied by Mitsubishi Materials Co., Tokyo,
Japan. These pellets were used for roomtemperature and high-temperature neutron diffraction measurements. Neutron
diffraction data were collected in air using HERMES [1], a diffractometer with a
150 multi-detector system, at room temperature and at high temperatures. The
HERMES is installed at the JRR-3M reactor in Japan Atomic Energy Agency, Tokai,
Japan. Neutrons with wavelength 1.8143
angstrom and 1.8207 angstrom were obtained by the (331) reﬂection of a Ge
monochromator. A furnace with MoSi2
heaters [2] was placed on the sample table,
and used for neutron diffraction measurements at high temperatures.
The experimental data were analyzed assuming the cubic perovskite-type structure(space group Pm-3m) by Rietveld methodwith a computer program RIETAN-FP [3].
La and Ba atoms were placed at the special position 1b 1/2, 1/2, 1/2 of the Pm3m symmetry. Co and O atoms were placedat the 1a 0, 0, 0 and 3d 1/2, 0, 0 sites, respectively. The calculated proﬁle agreed
well with the observed one (Fig. 1). The reﬁned crystal structure of La0.4Ba0.6CoO3-x
is similar with that of La0.6Sr0.4CoO3-x re-

ported in our previous work [4]. Analyeses
of diffraction data obtained at high temperatures are now in progress.
References[1] K. Ohoyama et al., Jpn. J. Appl. Phys. 37(1998) 3319.
[2] M. Yashima, J. Am. Ceram. Soc. 85(2002) 2925.
[3] F. Izumi and K. Momma, Solid State
Phenom. 130 (2007) 15.
[4] M. Yashima and T. Tsuji, J. Appl. Crystallogr., 40 (2007) 1166.

Fig. 1. Rietveld ﬁtting result for the neutrondiffraction data of La0.4Ba0.6CoO3-x measured atroom temperature.

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1-1-38Structural analysis of metavanadate phosphors AVO3 (A: K, Rb and Cs)
T. Nakajima1 , M. Isobe2 , T. Tsuchiya1 , Y. Ueda2 , and T. Kumagai1
1 Advanced Industrial Science and Technology, 1-1-1 Higashi, Tsukuba, 305-8565
2 Institute for Solid State Physics, Univ. of Tokyo, 5-1-5 Kashiwanoha, Kashiwa, 277-8581
Metavanadate phosphors AVO3 (A: K,
Rb and Cs) were ﬁrst discovered by Gobrecht et al. in 1957 [1]. The AVO3 shows abroad-band emission at 380 – 700 nm. We
have measured quantum efﬁciencies (η) of
these compounds; the η of KVO3 , RbVO3
and CsVO3 were 4, 59 and 80%, respectively. The origin of intense luminesecenceof the CsVO3 has not been disccussed wellin spite of its remarkable high value of η.
In this work, we have studied the powder
neutron diffraction for understanding luminescent properties of the AVO3 from theviewpoint of the structural features.
The polycrystalline samples of AVO3 (A:K, Rb and Cs) were prepared by a solidstate reaction. The powder neutron diffraction measurements for the obtained powder samples were performed using the
HERMES spectrometer installed at the research reactor JRR-3M in Japan Atomic Energy Agency, Tokai, Japan [2]. The wavelength of the incident neutron was selected
to be 1.8265 Å. The diffraction data werecollected in the 2θ range from 3 to 153 deg.
in the step interval of 0.05 deg. at room
temperature. The obtained data analyzed
by the Rietveld method using a computer
program RIETAN-FP [3].
Structural analysis of CsVO3 was carried out by using a reported structuralmodel, space group Pbcm [4]. The structural parameters were reﬁned as follows:a = 5.3979(3) Å, b = 12.2553(8) Å and c= 5.7881(3) Å. The reliability factors wereRwp = 4.97%, Re = 2.37%, RI = 2.89% and
RF = 1.54%. Main diffraction peaks were almost ﬁtted with the calculation result, however, the minor diffraction peaks can not beindexed by this structural model. In the
KVO3 and RbVO3 , the structural analyses
were also carried out, and the some minor
peaks were not indexed with Pbcm as simi-

lar with the case of CsVO3 .
For the discussion of luminescent properties of the AVO3 , the structural distortion
should be correctly determined, because
the emission intensity in these compounds
could strongly depend on the distortionof the VO4 tetrahedra in the crystal structure. In the conventional structural analysis using X-ray diffraction [4], the structural analysis of AVO3 was carried out using the space group Pbcm, and clear differences were not observed among the VO4tetrahedra of the AVO3 (A: K, Rb and Cs).
Therefore, unindexed peaks in this neutron
diffraction is expected to be a key point forthe discussion of the origin for luminescent
property of the AVO3 . The detailed structural analysis of these compounds are in
progress.
References[1] H. Gobrecht et al.: Z. Phys. 147 (1957) 350.
[2] K. Ohoyama et al.: Jpn. J. Appl. Phys. 37(1998) 3319.
[3] F. Izumi et al.: Mater. Sci. Forum 321-324(2000) 198.
[4] F. C. Hawthorne et al.: J. Solid State Chem.
22 (1977) 157.

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1-1-39Crystal structural change of potassium titanyl phosphate
Takafumi Komatsu, Masatomo Yashima, Takahiro Wakita, Yong Phat, Yoshitaka
Matsushita*
Department of Materials Science and Engineering, Interdisciplinary Graduate School of Scienceand Engineering, Tokyo Institute of Technology, * Quantum Beam Center, National Institute forMaterials Science
Nonlinear optical materials have received much attention in recent years.
Potassium titanyl phosphate (KTiOPO4 ,KTP) is one of them. The space group of
KTP is Pna21 at room temperature. KTP
exhibits a phase transition from ferroelectric to paraelectric phase at 1207 K. Second harmonic generation (SHG) effect disappears in the paraelectric phase. The crystal structure of the paraelectric phase of
KTP has not been investigated yet, probably due to the difﬁculty of diffraction experiments above 1000 K. The purpose ofthis work is to study the crystal structureof paraelectric phase of KTP using neutron
powder diffraction data measured at 1358
K.
A KTP sample was prepared by solidstate reactions at 1273 K for 3 hours. Neutron powder diffraction data were measured at 297, 639, 951, 1155, 1256 and1358 K using the HERMES diffractometer.
Wavelength of neutrons was 0.18265(1) nm.
Crystal structure of KTP was reﬁned by Rietveld method, using a computer program,
RIETAN-FP.
All the reﬂections observed in the diffraction data collected below 1207 K were indexed by the space group Pna21 , while
those measured above 1207 K were indexedby the space group Pnan. Figure 1 shows
the reﬁned crystal structure of paraelectric
KTP at 1358 K. The structure is characterized by helical chains of Ti06 octahedra thatare linked at two corners and are separated
by PO4 tetrahedra. The potassium ion is located in channel along the c-axis.
Unit-cell parameters a and b increased
with temperature up to 1358 K. The c parameter decreased with temperature up to1155 K and did not change largely above
the Currie temperature, 1207 K. The dis-placement of K atom along the c-axis decreased with an increase of temperatureand disappeared at and above 1207 K,
which indicates the displacive nature of theferroelectric-paraelectric transition. The
phase transition was also accompanied by
the change of occupancy factors at the Ksites, which indicates the order-disordernature of this transition.

Fig. 1. Reﬁned crystal structure of paraelectric
KTiOPO4 at 1358 K (space group Pnan).

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 582

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JAEA-Review 2011-050

1-1-40Li ion distributions of layered-structure type oxides LiNi1/2Mn1/2O2 prepared byion-exchange
Y. Arachi(A), H. Maeda(A), H. Kobayashi(B), T. Asai(A)(A) Kansai University, (B) AISTWe
have
extensively
investigated
Li2MnO3-based oxides with layered-NaCl
type to clarify the relationship between
crystal structure and electrochemical
property as cathode materials for Lithium
ion battery. LiNi1/2Mn1/2O2 is one ofthose and it exhibits a speciﬁc capacityof 150 mAh/g in the voltage range of 2.5
to 4.3 V. It is known that conventional
preparation produce about 10 % exchangeof Li and Ni in the layered-structure andthis Li/Ni disorder acts on increasing
the activation energy of Li migration andeffects on the cell performance[1,2]. We
have conﬁrmed that the phase transition
associated with cation ordering occurs
in discharged LiNi1/2Mn1/2O2.
The
objective of this study is to observe thechange of Li position by preparation condition and to determine lower temperature
structure as well. The samples wereprepared by ion-exchange of Li for Na
in NaN0.5Mn0.5O2. Neutron diffraction
measurement of the compositions is ofgreat useful to determine the ion distribution. It was performed by diffractometer,
HERMES installed at JRR-3M in the Japan
Atomic Energy Agency (JAEA) in Tokai,
Japan (JAEA). The wavelength of neutron
was 1.82646(6) . Diffraction data werecollected in the 2 θ range from 3 to 153
degree in the step interval of 0.1 degree.
Rietveld structural reﬁnement was carriedout by using a program RIETAN-2000 [3].
The obtained structure clearly depends on
the ion-exchange reaction temperature andtime. As increased reaction temperatureand time the Li/Ni disorder became remarkable. However, disordering of Li andNi was suppressed by this soft-chemical
process compared to those by conventional
preparation.
The obtained diffraction
patterns at 10 K will be applied for inter-

pretation of the magnetic behavior that
we have already observed a susceptibility
cusp at 15 K.
[1]Y. Arachi,H. Kobayashi, S. Emura, Y.
Nakata, M. Tanaka, T. Asai, H. Sakaebe, K.
Tatsumi and H. Kageyama, Solid State Ionics, 176, (2005)895-903.
[2] K. Kang, Y. S. Meng, J. Breger, C. P. Grey,
G. Ceder, Science, 311(2006)977.
[3] F. Izumi and T. Ikeda, Mater. Sci. Forum,
198 (2000) 321-324.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-1-41High temperature neutron diﬀraction study of (La0.9Sr0.1)MnO3+d perovskite
K. Nomura (A), H. Kageyama (A), K. Kakinuma (B), T. Maekawa (C), S. Nakamura (C),
H. Miyazaki (C), H. Imabayashi (C), and T. Ito (C)(A) National Institute of Advanced Industrial Science and Technology (AIST), (B) Kanagawa
University, (C) New Cosmos Electric Co., Ltd.
Strontium-doped lanthanum manganite perovskites, (La1-xSrx)MnO3+d havebeen investigated as the electrode materials of solid oxide fuel cells, because of thehigh electronic and relatively high oxideion conductivity [1]. However, the detailed crystal structures at elevated temperatures have not been reported yet. In thisstudy, we measured high temperature neutron diffraction data of 10 mol% Sr-doped
LaMnO3, (La0.9Sr0.1)MnO3+d (LSM), toinvestigate the crystal structure and the
conduction path of oxide-ions.
Neutron diffraction measurements were
performed in air with a 150-detector system, HERMES [2], installed at the JRR-3M
reactor in JAEA (Tokai). The neutron wave
length was 1.8265(1)A and the diffraction
data were collected in the 2 θ range from
20 to 153 deg in step interval of 0.1 deg, inthe temperature range from 297 to 1473K
and oxygen partial pressure, P(O2), range
between 2x10ˆ-4 and 0.21atm. A furnacewith Pt-Rh heaters installed in a vacuum
chamber was placed on the sample stage,and used for neutron-diffraction measurements at high temperatures. A tubulartype LSM sinter (outer diameter: 10 mm,
inner diameter: 7 mm, length: 50 mm) was
prepared, in order to obtain equilibrium
conditions between the sinter and atmospheres at short times. The diffraction dataobtained were analyzed using the Rietveld
program RIETAN-2000 [3]The diffraction data of LSM could be indexed assuming an orthorhombic symmetry (Pnma, No.62) (at 297 and 373K) or a
trigonal one (R-3c, No.167) (between 473
and 1473K) in P(O2) = 0.21 atm. Figure
1 shows the Rietveld reﬁnement result of
LSM measured at 1473K in P(O2) = 0.21
atm. The number of chemical formula perunit cell, reﬁned cell parameters, and reﬁned unit cell volume were as follows: z= 6, a = 5.6029(5)A, c = 13.679(2)A, V =371.87(7)Aˆ3. The reliability factors wereRwp = 5.51%, RI = 2.35%, and RF = 1.74%
Re = 2.96%. Goodness of ﬁt (S = Rwp/Re)
was 1.86.
References[1] N. Minh, J. Am. Ceram. Soc., 76, 563(1993).
[2] K. Ohoyama, T. Kanouchi, K. Nemoto,
M. Ohashi, T. Kajitani, and Y. Yamaguchi,
Jpn. J. Appl. Phys., 37, 3319 (1998).
[3] F. Izumi and T. Ikeda, Mater. Sci. Forum,
321-324, 198 (2000).

Fig. 1.
Rietveld reﬁnement result of(La0.9Sr0.1)MnO3+d at 1473K in P(O2) = 0.21
atm.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 595

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JAEA-Review 2011-050

1-1-42

Lithium Diﬀusion in LixFePO4
Atsuo Yamada, Shin-ichi Nishimura, Genki Kobayashi, Masatomo Yashima, Kenji
Ohoya
Ohoyma, Yasuo Yamaguchi
Tokyo Institute of Technology, Tohoku University
Chemical energy storage by batteries will
provide an important function in the future greener society. Lithium ion battery is
the most advanced energy storage systembut the application has been limited to theportable electronics devices due to the costand safety problems.
Neutron diffraction at high temperature as high as 350C was performed tounderstand the electrode reaction mechanism in the very important cathode material, LixFePO4, a use of which is now
widely recognized as the most promisingsolution to get lithium ion batteries into thelarge-scale application such as plug-in hybrid vehicles. For example, more than 200
papers have been published on this material last year.
Scientiﬁc community has raised theimportant question as to why facile redox reaction is possible in insulating material; the fact that the battery with insulating LixFePO4 electrode can deliver muchlarger current density than the battery withconventional metallic LixCoO2 electrode.
Geometric information on the movement ofcharge carrier should be the start point toanswer this important question.
By the careful analysis by maximum
entropy method, the long-awaited experimental evidence for one-dimensionallithium motion in LixFePO4 is displayed.
This provides fundamental knowledge toward full understanding the peculiar redox
mechanism.
Beyond LixFePO4, this is, to our knowledge, the ﬁrst visual demonstration of ionic
diffusion path in battery electrode.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 598

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JAEA-Review 2011-050

1-1-43

Soft modes in the relaxor ferroelectric compound (Na0.5 Bi0.5 )TiO3
M. Matsuura1 , H. Iida1 , K. Hirota1 , Y. Noguchi2 , and M. Miyayama2
1 Institute for Solid State Physics, The University of Tokyo, 106-1 Shirakata, Tokai, 319-1106
2 Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo
153-8505
waterfall feature observed in relaxor ferroelecrics Pb(Zn1/3 Nb2/3 )O3 -8%PbTiO3 [2]and Pb(Mg1/3 Nb2/3 )O3 . [3]References[1] J. Suchanicz and J. Kwapulinski, Ferroelectrics 165 249 (1995).
[2] P. M. Gehring et al., Phys. Rev. Lett. 84 5216
(2000).
[3] P. M. Gehring et al., Phys. Rev. Lett. 87
277601 (2000).
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&RXQWVPLQ(Na0.5 Bi0.5 )TiO3 (NBT) forms perovskite
structure with two different ions Na+ andBi3+ at the A site of ABO3 . NBT exhibitshigh and broad peak in the dielectric susceptibility which is very similar to that intypical relaxors and NBT regains attention
as promising applications to piezoelectric
devices containing no toxic lead. Last year,
we studied the diffuse scattering and clariﬁed that the diffuse scattering appears below about 800 K and has more intensity
along transverse direction than that along
longitudinal direction, suggesting a close
connection between the diffuse scatteringand soft transverse optical mode. The purpose of the present work is to study soft
phonon modes to clarify the mechanism of
the diffuse scattering in NBT. Neutron scattering experiments were performed on the
triple-axis spectrometers PONTA.
Figure 1(a) shows a constant-Q scan measured at Q =(2.05, 1.95,0) and T = 670 K.
The TO mode is strongly overdamped at
this Q and the spectra is well reproducedby broad lorentzian centered at ω = 0,
shown by the solid line. The TA mode is
not visible in panel (a) because its excitaton energy is below 2 meV. Figure 1(b) and(c) shows a similar constant-Q scan measured at Q =(2.15, 1.85, 0) and (2.25, 1.75, 0). In addition to clear peaks for TA modes,
a well-deﬁned peak for the TO mode wasobserved at 13 meV for (2.25, 1.75, 0) while
TO mode peak around 10 meV was rather
broad for (2.15, 1.75, 0). To investigate TA
and TO dispersions, a series of constant-Q
scans with a step of 0.05 rlu from q = 0 to
0.25 rlu and constant-E scans with a step of
1 meV from 6 to 11 meV were taken, andthe results are summarized in the inset toFig.2. No propagating mode was observedfor q < 0.10 rlu, indicating the so-called

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( PH9Fig. 1. Constant-Q scans measured at T = 670 K.
Panel (a) shows a damped TO mode for q = 0.05
rlu. Panels (b) and (c) show underdamped TA and
TO modes for q = 0.15 and 0.25 rlu. The inset shows
the TA and TO dispersions at T = 670 K.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 605

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JAEA-Review 2011-050

1-1-44
Anisotropic damping of transverse acoustic and optical modes in the relaxor
ferroelectric 0.7 Pb(Mg1/3 Nb2/3 )O3 -0.3 PbTiO3
M. Matsuura and K. Hirota
Institute for Solid State Physics, The University of Tokyo, 106-1 Shirakata, Tokai, 319-1106
comes underdaped, on the other hand, theTA mode for (2.15 1.85 0) becomes overdamped as shown in Fig.1(b) and (c). The
damped TA and TO modes were observedfor q =< 110 > directions which are thesame directions of the anisotropic diffuse
scattering. We speculated that PNR’s trap
soft phonon modes as a central peak. Besides, for the current case, PNR’s may trap
phonon modes anisotropically.
References[1] A. Naberezhnov et al. , Eur. Phys. J. B, 11,
13 (1999).
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Relaxor ferroelectrics have gained greatinterest recently due to their promising application as piezoelectric devices.
Pb(Mg1/3 Nb2/3 )O3 (PMN) is a typical relaxor which shows a broad and frequency
dependent peak in dielectric susceptibility. It is widely believed that the polar
nanoregions (PNR) occurring at temperatures much above Tc , the so-called Burns
temperature Td , play an important role insuch relaxor behavior. The lattice dynamics in PMN are characterized by a soft,zone center, transverse optic (TO) mode observed below Td , which is the so-called waterfall. Neutron scattering measurements
by Naberezhnov et al. on PMN revealed
the onset of strong diffuse scattering at orvery near Td ∼ 600 K [1], indicating a close
connection between the PNR and the diffuse scattering. Thus, it is expected thatthe local crystal distortion in PNR is driven
by the soft TO. To elucidate the lattice dynamics in PNR, we investigated low energy
phonon modes in PMN-30%PT. Neutron
scattering experiments were performed on
the triple-axis spectrometers HER installedat the JRR-3 Reactor of the JAEA.
Figures 1 show the constant Q spectrumat (2.15 1.85 0) and (2 -0.21 0) taken at
T = 600, 400, and 200 K. If the lattice dynamics is isotropic, these spectrum show
peaks for a transverse acoustic (TA) mode
and a transverse optical (TO) mode at thesame energies, because both Q’s locate at
the same q = 0.21 along the transverse
direction from each Bragg position. At
T = 600 K (> TC ), well-deﬁned TA and
TO modes were observed for (2 -0.21 0).
For (2.15 1.85 0), while the TA mode looks
very similar to that for (2 -0.21 0), the TO
mode is softer and broader in energy thanthat for (2 -0.21 0). Below TC , on the one
hand, the TO mode for (2.15 1.85 0) be-

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( PH9Fig. 1. Constant Q scan at (2.15 1.85 0) (closed circles) and (2 -0.21 0) (open circles) taken at T = 600,
400, and 200 K.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 606

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JAEA-Review 2011-050

1-1-45Behavior of Thermal Parameters through Phase Transition in KDP
H. Mashiyama, T. Miyoshi, T. Asahi and H. Kasano
Faculty of Science, Yamaguchi University, Yamaguchi 753-8512
KH2PO4 (KDP) is a well known ferroelectric (F) crystal which performs a phasetransition at 123K. Whether the proton istunneling or not in the paraelectric (P)phase has been controversial for a longtime. Moreover, the zero temperature structure in which all degrees of freedom arefrozen was not reported previously. Last
year we reﬁned the crystal structures down
to 15 K, by using neutron scattering.[1]However, the detailed measurement lacked
just around the transition temperature (Tc).
Here we report full results, especially thetemperature dependence of the DebyeWaller factor (U) through Tc.
A single crystal of KDP was set ina cryostat mounted on a diffractometer(FONDER) installed at JRR3M reactor in
JARERI, Tokai. Diffraction data up to
2theta<156 (neutron wave length 1.2452A)
were collected at two and three temperatures in phases P and F, respectively. Absorption and extinction correction was performed by using RADIEL. Atomic parameters were reﬁned by least-squared calculations.
Figure 1 shows atomic displacements in
the F phase. The PO4 tetrahedron deforms
abruptly at Tc with accompanying a relative displacement of K to induce dipole
moments. In the P phase, only proton takes
a mean structure (split atom). With decreasing temperature, all the thermal parameters U s decrease monotonically, with a tinychange at Tc, as shown in ﬁgure 2.
The extrapolated values of U to T=0
demonstrate the zero-point vibration of nuclei (ground state wave function). It should
be noted that the wave function of protonin the P phase is well described by superposing two ground state wave functions
with a separation of 0.3A. Since the proton density is almost single peak, proton
is considered to tunnel between two wells

frequently. Below Tc each proton links oneof two oxygen atoms to deform the PO4
tetrahedron. Comparing the magnitude of
U with the atomic displacement below Tc,
we can conclude that PO4 and K are notdisordered units in the P phase.
References[1] H. Mashiyama et al, ARNSR:ER Vol.14(2007) Num.96.
[2] R. J. Nelmes et al, J. Phys. C 15 (1982) 59.

Fig. 1. Atomic displacement along the c-axis of KDP.
Fig. 2 Temperature dependence of Debye-Waller
factor along the a-axis of KDP. The unit cell is referred to the P phase. The previous results after Ref.
[2] are shown by broken lines.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 608

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JAEA-Review 2011-050

1-1-46

Crystal Structure Analysis of Ferroelectric Niobium Oxides
N. Kumada, Y. Yonesaki, T. Takei,N.
N.Kinomura
KinomuraandandM.
M.Yashima*
Yashima*
University of Yamanashi and *Tokyo Institute of Technology
We performed the crystal structure reﬁnement of two types of perovskite-type oxides, Ba(Cu1/3Nb2/3)O3 and (Ba,H)BiO3
by using powder neutron diffraction data
which were collected in air with a 150detector system, HERMES, installed at JRR3M reactor in Japan Atomic Energy Research Institute (Tokai). High temperatureneutron diffraction data was collected byusing a furnace with MoSi2 heaters [1]which was placed on the sample table. The
data was reﬁned using the Rietveld methodwith the program RIETAN [2].
[1]Ba(Cu1/3Nb2/3)O3
Ba(Cu1/3Nb2/3)O3 has the perovskitetype structure with the tetragonal cellof a = 4.0218(4) and c = 4.1460(4) .
The structure reﬁnement by using neutron
diffraction data was carried out for two
types of models which have centrosymmetric P4/mmm(#123) and ancentrosymmetric P4mm(#99) space groups. The structure reﬁnement by using the centrosymmetric space group P4/mmm led to the Rfactors, Rwp =10.36, Rp = 7.60, RI = 3.17,
RF = 1.56%, S = 3.579, while by using ancentrosymmetric space group, P4mm thelower R-factors (Rwp = 8.96, Rp = 6.63, RI= 1.94, RF = 0.98%, S = 3.010) were obtained. This result suggested that this compound had an ancentrosymmetric spacegroup, P4mm. However, the displacementof z parameter for Ba and Nb atoms fromthat of O atoms was very small as shownin Fig. 1(a). We can not conclude that
this compound has an ancentrosymmetricspace group to exhibit ferroelectricity, andnow are attempting to improve the structure reﬁnement and to measure the electrical properties. This compound was foundto be transformed from the tetragonal to
cubic symmetry at 500 ˜ 600 °C. The structure reﬁnement of the high temperatureform by using neutron diffraction data was

successful leading to the R-factors, Rwp =9.82, Rp = 7.24, RI = 4.61, RF = 2.44%, S =2.900 in assumption with the space groupof Pm-3m (#221), and the lattice parameter
was a = 4.0957(3) . The crystal structureis shown in Fig. 1(b). Since this perovskitetype niobium oxide has a possibility of ferroelcricity, its crystal structure and electrical properties are now under investigation.
[2](Ba,H)BiO3
A new perovskite-type bismuth oxide,(Ba,H)BiO3 was prepared by hydrothermal
reaction using NaBiO3nH2O as a starting
compound. The X-ray powder diffraction
pattern of this compound could be indexed
withwith the cubic cell of a = 8.5445(4)the space group Pn3n(#222). The structure reﬁnement by using neutron diffraction data led to the reasonable R-factors,
Rwp = 8.72, Rp = 6.39, RI = 6.38, RF = 4.67%,
S = 2.358.
References[1] M. Yashima, J. Am Ceram. Soc.85 (2002)
2925.
[2] F. Izumi and T. IKeda, Mater. Sci. Forum
321 (2000) 198.

Fig. 1. Fig. 1 Crystal structure of BaCu1/3Nb2/3O3.
(a) low and (b) high temperature forms.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 612

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JAEA-Review 2011-050

1-1-47
Water Density Near Surface of DLC Films Having Various Surface Energies
Measured by Neutron Reﬂectometry
Tomoko Hirayama#1, Tomoki Uno#1, Takashi Torii#1, Takashi Matsuoka#1, Kazuko
Inoue#2, Toru Ebisawa#3, Seiji Tasaki#4, Masahiro Hino#5, Naoya Torikai#6#1Doshisha Univ., #2Waseda Univ., #3JAEA, #4Kyoto Univ., #5KURRI, #6KEKLubricants generally contribute to achieve
low friction on sliding surfaces in manykinds of mechanical components. It is wellknown that lubricants may form someabsorption layers near surfaces. Thoughmacroscopic relationships between lubricants (or absorption layers) and tribological properties have been studied everywhere, there are no reports on densities andthicknesses of the special ultrathin layers
formed at the solid-liquid interface.
In our laboratory, densities of lubricantsnear solid surfaces are directly measured
by neutron reﬂectometry and discussed in
the series of studies. The neutron can go
deeply into the inner region of common
metals because neutrons physically interact
not with electrons but with atomic nuclei,
thus the in-situ observations of solid-liquidinterface can be easily realized. The reﬂectometry is generally utilized for analysis ofvertical microstructures of a sample or theinterface through the reﬂectivity proﬁle. In
this paper, three kinds of DLC ﬁlms having
different surface energies were prepared
as base materials, and water was selected
as a lubricant. The DLC ﬁlms were called’normal DLC’, ’hydrophilic DLC’ and ’hydrophobic DLC’; the ﬁrst was deposited byplasma CVD using CH4 gas on a silicone
block, the second was treated by oxygengas plasma on the surface of the normal
DLC as post-processing treatment, and thethird was deposited by plasma CVD using
CH4 and C2F6. The DLC ﬁlms were soaked
in water in a specially-designed sample
holder, and the neutron beam was directly
entered to the DLC/water interface fromthe side of silicone block. Then, the instrument we used was a neutron reﬂectometer MINE in Japan Atomic Energy
Agency (JAEA), and the neutron reﬂectiv-

ity proﬁles from the interface between DLC
ﬁlms and water were obtained by the instrument. Through an analytical ﬁtting approach with Parratt s theory to the obtained proﬁles, we can see that: (1) the
thickness of hydrophilic layer (O2 plasma
treated layer) formed in the surface of hydrophilic DLC is 15nm, (2) water inﬁltrates from the surface to the interior of hydrophilic DLC until 15 nm-depth, and thethickness of dense water layer inﬁltrated in
the top surface of hydrophilic DLC is 2nm,
and (3) the thickness of low-density waterlayer on the surface of hydrophobic DLC is
3nm, and its density is almost half of normal water, shown in Fig. 1.

Fig. 1. Physical models estimated by neutron reﬂectometry

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 637

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JAEA-Review 2011-050

1-1-48Water Density Near Surface of DLC Films Having Various Surface Energies
Measured by Neutron Reﬂectometry
Tomoko Hirayama#1, Tomoki Uno#1, Takashi Torii#1, Takashi Matsuoka#1, Kazuko
Inoue#2, Toru Ebisawa#3, Seiji Tasaki#4, Masahiro Hino#5, Naoya Torikai#6#1Doshisha Univ., #2Waseda Univ., #3JAEA, #4Kyoto Univ., #5KURRI, #6KEKLubricants generally contribute to achieve
low friction on sliding surfaces in manykinds of mechanical components. It is wellknown that lubricants may form someabsorption layers near surfaces. Thoughmacroscopic relationships between lubricants (or absorption layers) and tribological properties have been studied everywhere, there are no reports on densities andthicknesses of the special ultrathin layers
formed at the solid-liquid interface.
In our laboratory, densities of lubricantsnear solid surfaces are directly measured
by neutron reﬂectometry and discussed in
the series of studies. The neutron can go
deeply into the inner region of common
metals because neutrons physically interact
not with electrons but with atomic nuclei,
thus the in-situ observations of solid-liquidinterface can be easily realized. The reﬂectometry is generally utilized for analysis ofvertical microstructures of a sample or theinterface through the reﬂectivity proﬁle. In
this paper, three kinds of DLC ﬁlms having
different surface energies were prepared
as base materials, and water was selected
as a lubricant. The DLC ﬁlms were called’normal DLC’, ’hydrophilic DLC’ and ’hydrophobic DLC’; the ﬁrst was deposited byplasma CVD using CH4 gas on a silicone
block, the second was treated by oxygengas plasma on the surface of the normal
DLC as post-processing treatment, and thethird was deposited by plasma CVD using
CH4 and C2F6. The DLC ﬁlms were soaked
in water in a specially-designed sample
holder, and the neutron beam was directly
entered to the DLC/water interface fromthe side of silicone block. Then, the instrument we used was a neutron reﬂectometer MINE in Japan Atomic Energy
Agency (JAEA), and the neutron reﬂectiv-

ity proﬁles from the interface between DLC
ﬁlms and water were obtained by the instrument. Through an analytical ﬁtting approach with Parratt s theory to the obtained proﬁles, we can see that: (1) the
thickness of hydrophilic layer (O2 plasma
treated layer) formed in the surface of hydrophilic DLC is 15nm, (2) water inﬁltrates from the surface to the interior of hydrophilic DLC until 15 nm-depth, and thethickness of dense water layer inﬁltrated in
the top surface of hydrophilic DLC is 2nm,
and (3) the thickness of low-density waterlayer on the surface of hydrophobic DLC is
3nm, and its density is almost half of normal water, shown in Fig. 1.

Fig. 1. Physical models estimated by neutron reﬂectometry

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 638

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JAEA-Review 2011-050

1-1-49Magnetic structure of Pr2-2xCa1+2xMn2O7(x=0.45)
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Bilayermanganite
Pr22xCa1+2xMn2O7(x=0.5) is a CE-type
antiferromagnet with TN=143 K [1].
To study the robustness of the CE-AF
state against the change of the holeconcentration, we have examined the Pr22xCa1+2xMn2O7(x=0.45) system. Single
crystal of Pr2-2xCa1+2xMn2O7(x=0.45)
was prepared by ﬂoating-zone method.
Neutron scattering measurements werecarried out with the triple axis spectrometer GPTAS installed at JRR-3M.
The measurements were done on thepseudo-tetragonal (hhl) reciprocal zone.
Figure (a) shows the results of q=(1/4,
1/4, l) scan taken at 200 K and 3 K. In thecase of x=0.5, strong magnetic reﬂections
are observed at l=integer positions, which
results from CE-AF (see inset). For x=0.45,
only diffuse scattering is observed even at 3
K, indicating that the correlation of the CEtype AF in this system is a shot-range one.
Results of q=(h, h, 3) scan (Fig. (b)) suggest the anisotropic nature of the magnetic
correlation. Figure (c) shows the temperature dependence of the diffuse intensity at
q=(1/4, 1/4, 3). The intensity starts to increase below 120 K as decreasing temperature. These results are consistent with themagnetization and resistivity data.
Pr2-2xCa1+2xMn2O7 is the 2D analog of the similar minimal-disorder system of perovskite Pr1-xCaxMnO3. However, results of neutron diffraction measurements indicate the robustness of the
CE-AF state against the change of the holeconcentration is quite different from Pr1xCaxMnO3, where long-range CE-AF isstable for x>0.3.

 

Y. Tokunaga(A), D. Okuyama(A), T.J. Sato(B), T. Arima(C), and Y. Tokura (A,D)
ERATO-MF, JST(A), ISSP, Univ. of Tokyo(B), IMRAM, Tohoku Univ.(C), Dept. Appl. Phys,
Univ. of Tokyo(D)

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Fig. 1. Proﬁles of CE-type spin order observed
along (a) q=(1/4,1/4,l) and (b) (h,h,3). (c) Temperature dependence of the diffuse intensity observed
at q=(1/4,1/4,3).

[1] Y. Tokunaga et al, to be published in
PRB.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 649

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JAEA-Review 2011-050

1-1-50

Neutron scattering in Ising-like one dimensional antiferromagnet BaCo2 V2 O8
T. Masuda, S. Hondo, and M. Matsuuraa
International Graduate Schools of Arts and Sciences, Yokohama City University,
22-2 Seto, Kanazawa-ku, Yokohama, 236-0027
a Neutron Scattering Laboratory, Institute for Solid State Physics,
University of Tokyo, 106-1 Shirakata, Tokai, Ibaraki, 319-1106, Japancylindrical shape with φ8 mm × 20 mm.
The chain axis is crystallo graphical c direction and we put scattering plane as (h 0 l ).
We performed a series of constant q
scans. Well deﬁned peaks were observed
as is shown in the typical scan in Fig. 1.
The boundary energy is 7 meV and theanisotropy gap is 2 meV that are consistent
with theoretical calculation. Since Co ionsform 4-folded screw chain, four modes are
predicted of which two modes are degenerated. Doing Fourier transformation of the
Co position we obtained the structure factor with the modulation in a∗ - b∗ plane. By
selecting adequate q we obtained a set ofscans free of additional mode. The magnetic dispersion is mostly consistent withtheory. Further analysis and calculation
will appear in forthcoming paper.
References[1] S. Kimura et al., Phys. Rev. Lett. 99,
087602 (2007), S. Kimura et al., Cond-mat
0707.4713.
5G PONTA
36'-40'-sample-PG-40'-80'

Intensity (Counts/3 min.)In one-dimensional antiferromagnetic
XXZ model the phase diagram of theground state contains characteristic nature of quantum ﬂuctuation: Néel state< 1, quantum criticality at= 1,in> 1. Hereisand spin liquid at
XXZ anisotropy parameter. In the uniform magnetic ﬁeld characteristic behavior of Tomonaga-Luttinger liquid is identiﬁed by incommensurate spin correlation
in longitudinal mode. Recently such experimental realization was discovered in
BaCo2 V2 O8 [1] by the combination of magnetization, ESR, and heat capacity measurements. The compound shows usualNéel transition at 5.4 K in zero ﬁeld. In applied ﬁeld at h > 4 T a new phase appears
at T < 1.4 K which could be concernedwith incommensurate spin correlation. The
study of the spin dynamics by neutron scattering technique in BaCo2 V2 O8 is a matterof importance. Eventually we noticed that
another group in Europe is proceeding thesimilar study. We think that this study has
priority over the original proposal titled“neutron scattering study in O2 adsorbed
CPL-p1.” Hence we performed inelastic
neutron scattering study in BaCo2 V2 O8 inzero ﬁeld in the 8th cycle in the ﬁscal yearof 2007.
From the previous studies it is estimated= 0.53, and J  =that J = 5.4 meV,−0.065J. Here J is the intrachain interaction and J  is the next nearest neighbor
intrachain interaction. Exact diagonalization calculation predicts the anisotropy gapof 1.55 meV and the boundary energy of
7meV. Therefore we select thermal neutron
with tight collimation setup: 36’ - 40’ - sample - PG - 40’ - 80’ with ﬁxed ﬁnal energyof E f = 13.5 meV. The prepared crystal is

E =13.5 meV
f

200

100

0

( 3 0 0)

0

2

4

6

8

10

12

14

16

Energy transfer (meV)Fig. 1. Typical constant q scan in BaCo2 V2 O8

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 652

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JAEA-Review 2011-050

1-1-51

Crystal structural analysis of rutile-type titania

Yong Phat, Masatomo Yashima, Takahiro Wakita, Takafumi Komatsu
Department of Materials Science and Engineering, Interdisciplinary
Graduate School of Science, Tokyo Institute of Technology
Titanium dioxide (titania) is a technologically important material with applications
in photocatalysis, paints, gas sensors, electrochromic devices, lithium ion batteries,
and dye-sensitized solar cells. TiO2 crystallizes most commonly in either the rutile (space group P42/mmm) or anatazetype structure. For bulk titania crystals atambient conditions, rutile is more stable
than anatase and has therefore been more
widely studied. In contrast to the extensive
studies on its crystal structure, however
structural properties of the rutile structure
in high temperature have not been studied
in detail and not well understood. In thisstudy, we investigated the crystal structure of rutile-type titania at high temperatures by using neutron powder diffraction
method.
Rutile-type titania powders were pressed
into pellets. These pellets were used forhigh-temperature neutron diffraction measurements. Neutron diffraction measurements were performed in air with a 150detector system, HERMES [1], installed at
the JRR-3M reactor in Japan Atomic Energy Agency, Tokai, Japan. Neutrons with
were obtained bywavelength 1.8143
the (331) reﬂection of a Ge monochromator. Diffraction data were collected in air
from room temperature to high temperatures. A furnace with MoSi2 heaters [2] wasplaced on the sample table, and used forneutron diffraction measurements at hightemperatures. The experimental data wereanalyzed by a combination of Rietveld
analysis, the maximum-entropy method(MEM) and MEM-based pattern ﬁtting(MPF). Computer programs RIETAN-FP,
PRIMA and VESTA were utilized for the
Rietveld and MPF analyses, MEM calculation and visualization of crystal structureand nuclear-density distribution, respec-tively. The data analysis is now in progress.
Reference[1] K. Ohoyama et al., Jpn. J. Appl. Phys. 37(1998) 3319.
[2] M. Yashima, J. Am. Ceram. Soc. 85(2002) 2925.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 661

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JAEA-Review 2011-050

1-1-52Diﬀuse Scattering of PbF2

Xianglian, K. Basar, S. Siagian, T. Sakuma, H. Takahashi1 and N. Igawa2
1

Institute of Applied Beam Science, Ibaraki University, Mito 310-8512
Institute of Applied Beam Science, Ibaraki University, Hitachi 316-8511
2
Japan Atomic Energy Agency, Tokai 319-1195

Diﬀuse scattering contains information
about a short-range-order in a disorderedarrangement (static disorder) and thermal
vibrations of atoms (thermal disorder) in
crystals1) . The oscillatory diﬀuse scattering
intensities were observed from ordered crystals at room temperature due to the correlation eﬀects among thermal displacements ofatoms2) . High temperature phase of PbF2
is known as a superionic conductor with anion disorder. In order to clarify the inﬂuenceof the correlation eﬀects among thermal displacements of atoms and the disorder of anions, the neutron diﬀuse scattering proﬁle in
PbF2 was studied.

scattering intensity at 773 K includes the contribution from disordered arrangements of F
atoms and thermal vibrations of atoms.

Neutron scattering measurements were performed on powder PbF2 at 295, 633 and 773
K by HRPD. Powder samples were set in a
vanadium container of 10 mm in diameter. Incident neutron wavelength was 1.823 Å. The
scattering data were collected in the range ofscattering angle from 10◦ to 160◦ with step
angle 0.05◦ . The observed diﬀuse neutron
scattering intensities of PbF2 are shown by
broken lines in Fig. 1.
Rietveld reﬁnement analysis has been performed on the neutron scattering intensities of
PbF2 . Room temperature phase of PbF2 belongs to orthorhombic system. The phase of
PbF2 at 633 K belongs to cubic system. The
phase of PbF2 at 773 K also belongs to cubic system and has disordered arrangementsof F atoms. The calculated diﬀuse scattering intensities are shown by solid lines in Fig.
1. The values of correlation eﬀects were included in the calculation for the interatomic
distances less than 5 Å. The other values ofcorrelation eﬀects are assumed to be 0. The
observed diﬀuse scatterings at 295 and 633
K are explained by correlation eﬀects among
thermal displacements of atoms. The diﬀuse
原子炉：JRR-3

装置：HRPD(1G)

Figure 1: Neutron scattering intensities of powder
PbF2 above room temperature.

References
1) T. Sakuma: J. Phys. Soc. Jpn.”, 62, pp. 41504151 (1993).
2) T. Sakuma et al.: Solid State Ionics”, 176, pp.
2689-2693 (2005).

分野：中性子散乱（構造）㻙㻌 㻤㻠㻌㻙

JAEA-Review 2011-050

1-1-53Structural Features of Lithium Ion Conductor Li1+x Ge2−x Alx (PO4 )3
Y. Fujita, H. Takahashi, T. Sakuma1 and N. Igawa2
Graduate School of Science and Engineering, Ibaraki University, Hitachi, Ibaraki 316-8511
1Graduate School of Science and Engineering, Ibaraki University, Mito, Ibaraki 310-8512
2
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

LiGe2 (PO4 )3 is a inorganic compound thathas a so-called NASICON-type structure andindicates high Li+ ion conduction. The substitution of Ge4+ ions by Al3+ ion leads tothe increase of Li+ ion concentration so thatthe charge neutrality in the compound is held.
The chemical formula for Al-substituted compound is expressed as Li1+x Ge2−x Alx (PO4 )3 ,denoted as Al-LISICON. The space group of
Al-LISICON is R-3c. The ionic conductivity
increases with Li+ ion concentration. In thiscase, excess Li+ ions expressed by x in thechemical formula are distributed on 18e site.
It has been reported that substituted Al3+ ion
does not occupy Ge site but P site by NMR
investigation 1) . In the present study, X-ray
and neutron diﬀraction experiments were performed to clarify the characteristic featuresof the crystal structure for Al-LISICON at
x =0.5. Neutron diﬀraction was done at 10,
150 and 300K by HRPD installed in JRR3M. Diﬀraction pattern from HRPD at 300
K is shown in Fig. 1. Based on the Rietveld
analysis, it is suggested that substituted Al3+ion is distributed only on Ge site. It is known

that strong diﬀuse scattering is observed especially in superionic conductors. Remarkable
thermal diﬀuse scattering is expected in thediﬀraction proﬁle of Al-LISICON, because ofhigh Li+ ion conduction in this compound.
However the diﬀuse scattering intensity highlighted in the inset in Fig. 1 is almost thesame as those in 150 and 10 K. These results suggest that the most of the diﬀuse scattering comes from not the thermal motion
but the static disorder of constituted ions.
Alami et al. reported that Li+ ion at 6bsite is slightly displaced to (001) direction in
LiGe2 (PO4 )3 2) . Our structure reﬁnement using Rietveld analysis gives unsatisfactory result at present. One of the reasons might arise
from static disorder of Li+ ions. More detailed analysis for Li+ ion distribution in AlLISICON is in progress.
References
1) P. Maldonado-Manso, M. C. Martin-Sedeño, S.
Bruque, J. Sanz and E. R. Losilla :“Solid State
Ionics”, 178, 43(2007).
2) M. Alami, R. Brochu, J. L. Soubeyroux, P. Gravereau,
G. Flem and P. Hagenmuller :“J. Solid State Chem.”,90, 185(1991).

Figure 1: Neutron diﬀraction proﬁle for Li1.5 Ge1.5 Al0.5 (PO4 )3 at 300 K. The inset shows an expansion of thediﬀuse background portion.

原子炉：JRR-3

装置：HRPD(1G)

分野：中性子散乱（構造）㻙㻌 㻤㻡㻌㻙

JAEA-Review 2011-050

1-1-54
Xe Motion in Clathrate Deuterohydrate Analyzed by Applying
Rietveld/Maximum Entropy Method
N. Igawa, T. Taguchi, H. Fukazawa, H. Yamauchi, W. Utsumi and Y. Ishii1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Radiation Application Development Association, Tokai, Ibaraki 319-1106

Xenon hydrate is a structure I type
clathrate hydrate at the atmospheric pressure and below the decomposed temperature.
Although the three dimensional hydrogenbonded framework in clathrate hydrate had
been reported, the details of Xe gas motions in
the framework are not clear. In this study, we
analyzed the scattering length density distribution of Xe deuterohydrate by Rietveld andMEM analysis of neutron powder diﬀraction
data to clarify the Xe motion.
We prepared deuterohydrate for the neutron diﬀraction to suppress the incoherent neutron scattering, which are especiallycaused by the H atoms. Neutron powder
diﬀraction measurements were carried out using the HRPD at the temperatures of 10,
115, and 245 K. A neutron wavelength of
0.1823 nm was used. Crystal structures
were determined from the diﬀraction patterns by the Rietveld method using the proAfter the Rietveld
gram “RIETAN-FP”.1)
analysis, the scattering density distribution
maps were analyzed by applying the maximum entropy method analysis using the program “PRIMA”.2)
Figure 1 shows a result of Rietveld reﬁnement at 10 K. All peaks were from the Xe
deuterohydrate, and no reﬂections of impurities were observed. The R wp and S are
3.42 % and 1.10. Structure I hydrates consist of 46 ice molecules in a framework of
two dodecahedral cages (small cages) and six
tetrakaidecahedral cages (large cages) in aunit cell. Figure 2 shows the temperature dependence of the scattering length density distribution maps of the small and large cagesof Xe deuterohydrate. All maps were drawn
with the same isosurface level, 1.0 fm/Å3 . In
the small cage, a spherical positive scattering
length density was observed at the center of
原子炉：JRR-3

装置：HRPD(1G)

the cage, which is attributed to Xe. An ellipsoid shaped scattering length density distribution at the center of the cage was observedin the large cage; the major axis of the density
distributuion was directed toward the centerof a hexagonal facet of the large cage. The
distributions of Xe in the both cages were almost the same at any temperature.

Figure 1: The result of the Rietveld analysis of Xe
deuterohydrate at 10 K.

Figure 2: Scattering length density distribution maps
for diﬀerent temperatures.

References
1) F. Izumi et al.:“Solid State Phenom.”, 13015(2007).
2) F. Izumi et al.:“Recent Research Development inPhysics II”, 3, 699(2002).

分野：中性子散乱（構造）㻙㻌 㻤㻢㻌㻙

JAEA-Review 2011-050

1-1-55
Neutron Powder Diﬀraction and Diﬀerence MEM Analysis ofProtium- and Deuterium-Dissolved BaSn0.5 In0.5 O2.75+α
T. Nagasaki1 , S. Shiotani2 , M. Yoshino2 , K. Iwasaki2 ,N. Igawa3 , H. Fukazawa3 and W. Utsumi3
1

2

EcoTopia Science Institute, Nagoya University, Nagoya 464-8603
Department of Materials, Physics and Energy Engineering, Graduate School of Engineering,
Nagoya University, Nagoya 464-8603
3
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Some perovskite oxides with dopant cations
and oxide ion vacancies absorb water vapor in
humid atmosphere to release mobile hydrogenions (protons) into the structure, thereby becoming proton conductors. These materials
are of fundamental interest as well as of practical one because of their potential applications to protonic devices including fuel cells.
Recently maximum entropy method(MEM) combined with neutron powder
diﬀraction has been extensively used toinvestigate the crystal structures of ionic
conductors including
proton-conducting
oxides 1–3) . It is because in general, theMEM is eﬀective for revealing static anddynamic disorder in crystals. However, as
we pointed out in the previous paper 4) , thespatial resolution of 3D atomic distribution
map deduced by MEM is limited especiallywhen the neutron wavelength is long and theatomic concentration is low.
Therefore, we introduced a new method,
the diﬀerence MEM analysis of neutron
diﬀraction data, as a method to reveal detailed structure around hydrogen atoms inproton-conducting oxides. It is a MEM analysis of the diﬀerences between the structure
factors of protium- and deuterium-dissolved
crystals. Simulation has demonstrated that it
not only provides the distribution of hydrogen atoms alone but also improves the spatial
resolution of the MEM mapping around hydrogen atoms.

distribution or diﬀusion pathways of atoms.)
In the diﬀerence MEM analysis, however, we
locate hydrogen atoms and other atoms inseparate MEM calculations. In other words,
they are not neighboring during the MEM calculations. That is why the diﬀerence MEM
analysis drastically improves the separation
between hydrogen and other atoms.
The diﬀerence MEM analysis was then applied to actual neutron diﬀraction dataofprotiumand
deuterium-dissolved
BaSn0.5 In0.5 O2.75+α . The result (Fig. 1,
right) shows that O-H bonds mostly tilt
towards the second nearest oxygen atoms andthat distribution of hydrogen and/or oxygen
atoms are insigniﬁcant in interstitial regions .

Figure 1: Scattering length density distributions in
D2 O-dissolved BaSn0.5 In0.5 O2.75+α deduced by theordinary MEM analysis (left) and the diﬀerence MEM
analysis (right). RIETAN-FP, PRIMA and VESTA
were used for the analysis and the drawing.

References

It should be noted that the MEM mapping
in its own nature has a tendency to connect
and merge the neighboring areas in the 3D
atomic distribution. (We must take this behaviour into account when discussing minor
原子炉：JRR-3

装置：HRPD(1G)

1) T. Ito, T. Nagasaki et al. :“Solid State Ionics”,
178, pp. 607-613 (2007).
2) X. Kuang et al. :“Nature Mater.”, 7, pp. 498-504(2008).
3) S. Nishimura et al. :“Nature Mater.”, doi:10.1038/
nmat2251 (2008).
4) T. Nagasaki et al. :“J. Nucl. Sci. Technol.”, Suppl.
5, in print (2008).

分野：中性子散乱（構造）㻙㻌 㻤㻣㻌㻙

JAEA-Review 2011-050

1-1-56In Situ Powder Neutron Diﬀraction Experiment under High Pressure
W.Utsumi, K.Komatsu1 , H.Arima1 , H.Kagi1 , T.Okuchi2 ,S.Sasaki3 , H.Yamauchi, H.Fukazawa, N.Igawa and T.Kamiyama4
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Graduate School of Science, The Tokyo University, Hongo, Bunkyo-ku, Tokyo 113-0011
2
Institute for Study of the Earth’s Interior, Okayama University, Misasa, Tottori 682-0193
3
Department of Materials Science and Technology, Gifu University, Yanagido, Gifu 501-1193
4High Energy Accelerator Research Organization (KEK), Oho, Tsukuba, Ibaraki 305-0801
1

Application of high pressure to materials
often induces drastic changes in structure,physical properties, chemical reactions, etc.,
and sometimes remarkable phase transitions
may occur. It is expected that high pressurematerial science and the investigation of the
Earth s interior will greatly improve using
the high ﬂux pulse neutrons of J-PARC. We
carried out a preliminary test experiment using the High Resolution Powder Diﬀractometer (HRPD) at JRR-3 to check the feasibilityof the high pressure device1) .
A Paris-Edinburgh cell, which is a standard
high pressure device for the neutron experiment in Europe and USA, was mounted on
the rotation stage of HRPD (Figure 1). A pairof anvils made of cubic born nitride (cBN)was used for the pressure generation. Diﬀraction proﬁles of Pb (initial size: 6mm in diameter and 1.6mm in height) placed in the highpressure cell were observed at 0 GPa (ambient conditions) and 2.9 GPa (applied load
was 30 ton). Incident and diﬀracted neutron
beams (wavelengh:1.823Å) pass through theanvil gap which is perpendicular to the compression axis. The exposure time was 2 and10.5 hours for ambient and at high pressures,
respectively.
Figure 2 shows the diﬀraction proﬁles thus
obtained. Several peaks of Pb were clearlyobserved and the calculated lattice constants
at 0 GPa and 2.9 GPa were 4.9518(3) and
4.8746(3) Å, respectively. Although the sample was surrounded by gasket and anvil materials, the background noise signals from thesematerials were reduced signiﬁcantly due to
原子炉：JRR-3

装置：HRPD(1G)

the ﬁne collimation of HRPD and the use ofcBN anvils. Present results provide us useful information for the in situ high pressure
experiments at J-PARC.

Figure 1: Paris-Edinburgh cell mounted on HRPD.

Figure 2: Diﬀraction proﬁles of Pb at 0 and 2.9 GPa.

References
1) K.Komatsu, H.Arima, H.Kagi, T.Okuchi, S.Sasaki,
H.Yamauchi, H.Fukazawa, N.Igawa, W.Utsumi,
and T.Kamiyama:“A high pressure experiment of
powder neutron diﬀraction on the HRPD at JRR3”, Rev. High Press.Tech.(Japanese), 18, 170(2008).

分野：中性子散乱（構造）㻙㻌 㻤㻤㻌㻙

JAEA-Review 2011-050

1-1-57
Pressure-Temperature Phase Diagram of Filled Skutterudite PrFe4 P12
T. Osakabe and K. Kuwahara1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Graduate School of Science and Engineering, Ibaraki Univ., Mito, Ibaraki 310-8512

Filled skutterudite compound PrFe4 P12shows a Γ1 -type electronic mulitipolar order
below TA = 6.5 K at ambient pressure 1, 2) .
The propagation vector is q = (1, 0, 0), which
is closely related with the nesting property of
the Fermi surface 3) . Applied pressure suppresses this orderd phase (A-phase, hereafter)
and induces an insulating phase above 2.4
GPa at low temperature 4) .
We performed neutron diﬀraction experiments under hydrostatic pressure up to 4.3
GPa to investigate the order parameter in thepressure-induced insulting phase. The experiments were carried out by using the TAS1 spectrometer in JRR-3, JAEA at Tokai.
The high pressure was generated by a newlydeveloped hybrid-anvil device composed ofa large sapphire anvil and a tungsten carbide anvil 5) . Glycerin was employed as apressure-transmitting medium, which transmits the hydrostatic pressure at least up to 7
GPa 6) . The sample size was about 0.8 ×0.6
×0.2 mm3 .
Above 2.7 GPa, we found the AFM orderwith the propagation vector of q = (1, 0, 0),
which is identical with that in the A-phase.
The N éel temperature and ordered magnetic
moment per Pr ion are summarized in ﬁg. 1
as a pressure-temperature phase diagram together with the data in ref. 4) . As shown inﬁg. 1, the AFM ordered phase (M-phase, hereafter) corresponds to the pressure-induced insulating phase and highly stabilized by applied pressure. The magnetic structure in
the M-phase is schematically shown in ﬁg. 1.
The transition from the A-phase to the Mphase is ﬁrst order. The magnetic moment at
1.5 K is approximately 2.0 μB , which is consistent with the dipole moment in the CEF(1)ground state of the Γ1 -Γ4 with d ∼ 1 quasiquartet 7, 8) . The drastic change in the order parameter from the A-phase to the M原子炉：JRR-3

装置：TAS-1(2G)phase at relatively low pressure is suppose to
be originated from the comparable ordering
energy between the multipoles in the highly
degenerate ground state in this compound.

Figure 1: Pressure-temperature phase diagram of
PrFe4 P12 .

References
1) Y. Aoki, T. Namiki, T. D. Matsuda, K. Abe, H.
Sugawara, and H. Sato :,“Phys. Rev. B”, 65, pp.
064446-1-7 (2002).
2) J. Kikuchi, M. Takigawa, H. Sugawara, and H.
Sato : “J. Phys. Soc. Jpn.”, 76, pp. 043705-1-4(2007).
3) H. Harima, K. Takegahara, S. H. Curnoe, K. Ueda
: “J. Phys. Soc. Jpn.”, 71 Suppl. pp. 70-73 (2002).
4) H. Hidaka, I. Ando, H. Kotegawa, T. Kobayashi,
H. Harima, M. Kobayashi, H. Sugawara and H.
Sato :“Phys. Rev. B”, 71, pp. 073102-1-4 (2005).
5) T. Osakabe, K. Kakurai, D. Kawana and K. Kuwahara : “J. Magnetism Magnet. Mater.”, 310, pp.
2725-2727 (2007).
6) T. Osakabe and K. Kakurai :“Jpn. J. Appl. Phys.”,47, pp. 6544-6547 (2008).
7) A. Kiss and Y. Kuramoto :“J. Phys. Soc. Jpn.”,
74, pp. 2530-2537 (2005).
8) Y. Kuramoto, A. Kiss, J. Otsuki and H. Kusunose:“J. Phys. Soc. Jpn.”, 75 Suppl. pp. 209-214 (2006).

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JAEA-Review 2011-050

1-1-58
Cu Dimer Excitations in Cu2 Fe2 Ge4 O13
T. Masuda and K. Kakurai1
1

Yokohama City University, Yokohama, Kanagawa 236-0027
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Cu2 Fe2 Ge4 O13 is a rare experimental realization of weakly coupled quantum dimers(Cu) and classical chains (Fe) compound 1) .
So far Fe centered magnetic excitations inlower energy range, which can be explained byweakly coupled Fe spins, had been studied indetail. For example, careful measurement of
the magnetic dispersion in LTAS spectrometer revealed the existence of eﬀective magnetic
interaction by way of non-magnetic singlet Cu
dimer 2) .

neutron cross section based on dimers in staggered and random ﬁelds, respectively. Excellent agreements between the experiment andcalculation mean that the proposed eﬀective
spin models are realized in Cu2 Fe2 Ge4 O13 .

From the view of Cu dimers diﬀerent typeof eﬀective models would be realized, namely
Cu dimers in the staggered ﬁeld from neighboring Fe moments at T < TN and dimers in
random ﬁeld at T > TN . Such models haverarely been realized in external zero magnetic
ﬁeld. To verify the models in Cu2 Fe2 Ge4 O13
we measured Cu centered dispersionless modeat ω ∼24meV on TAS1 in JRR-3M.
Figure (a) is constant q scans in diﬀerent
temperatures. Well deﬁned peaks due to Cu
dimers are observed at ω = 24 meV. At
7 K the peak is within resolution indicatedby gray area. With the increase of temperature the width becomes wider and at T >54K
(well above TN ) it reaches the saturation. The
behaviors are qualitatively explained by density of state (DOS) of triplet excitations ofspin dimers in staggered/random ﬁeld. In
the staggered ﬁeld the triplet splits into singlet√and doublet with E√doublet = 1/2J +1/2 4h2 + J 2 , Esinglet = 4h2 + J 2 . In random ﬁeld the triplets split intro the energy
range of J −h < E < J +h. Here h is the ﬁeld
scaled in energy (h = gμB H). Because h (5.48
meV) is small compared with J (J = 24 meV)[1] the DOS in the latter spreads in wider energy range than that in the former. Consequently the excitation in constant q scans at
T > TN becomes broad. The dotted and bold
solid curves are the theoretical calculations of
原子炉：JRR-3

装置：TAS-1(2G)

References
1) T. Masuda et al., PRL 93, 077202 (2004).
2) T. Masuda et al., PRB 75, 220401(R) (2007).

分野：中性子散乱（構造）㻙㻌 㻥㻜㻌㻙

JAEA-Review 2011-050

1-1-59Local Lattice Distortion in Giant Negative Thermal Expansion Material
Mn3 Cu1−x Gex N
S. Iikubo, K. Kodama, K. Takenaka2,3 , H. Takagi3,4 and S. Shamoto
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Department of Crystalline Materials Science, Nagoya University, Nagoya 464-8603
3
RIEKN (T heInstituteof P hyscalandChemicalResearch), Wako, Saitama 351-0198
4
CREST , Japan Science and Technology Agency, Kawaguchi, Saitama 332-0012
1

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Figure 1: Main panel : T -dependence of the intensityof magnetic (100) reﬂection for x=0.15, 0.5 and 0.7.
Inset : T -dependence of the lattice constant.

tice constant from diﬀraction data. These results indicate that in the sample whose lattice
constant gradually increases with decreasing
T , the magnitude of the ordered moment
gradually increases.
Figure 2 shows atomic pair distributionfunctions G(r) of Mn3 Cu1−x Gex N obtained
from pulsed neutron diﬀraction data collected
原子炉：JRR-3

装置：TAS-2(T2-4)

on the powder diﬀractometer NPDF at theLos Alamos Neutron Science Center. Peak (1)) T  CTDWPKVU

Mn3 Cu1−x Gex N exhibits sharp magnetovolume eﬀect (MVE) for x ∼ 0.15, and withincreasing x, MVE becomes broad against
temperature (T ), similar to Invar eﬀect, leading to a giant negative thermal expansion
coeﬃcient1) . Previous neutron diﬀraction
measurement indicates that the system which
exhibits large MVE (0.15 ≤ x ≤ 0.7), hasso-called Γ5g -type antiferromahentic orderingand the structure remains cubic below TN 2) .
In this study, we performed powder neutron
diﬀraction on Mn3 Cu1−x Gex N to investigate
the mechanism of the broadening of MVE.
T -dependence of the scattering intensity ofmagnetic (100) reﬂection is shown in main
panel of Fig. 1. The intensity is normalized
by the intensity of nuclear (100) reﬂection.
The inset shows the T -dependence of the lat-

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Figure 2: Atomic pair distribution functions G(r) of
Mn3 Cu1−x Gex N for x=0.7, 0.5 and 0.15 at 300 K.

indicates atomic correlation between Mn and
N in Mn6 N octahedron. Peak (2) is a superposion of negative Mn-Cu (Ge) and positive
Mn-Mn correlations. Peak (1) is a sharp single peak. In contrast, peak (2) splits into two
peaks (shown by arrows). These indicate that
Mn-octahedron rotates without the change ofthe shape. Although the periodic rotation of
Mn-octahedron causes the structural transition to tetragonal structure in Mn3 GeN, theaverage strcuture of these samples remain cubic, indicating that the rotation is not periodic. It is found that the local Mn-octahedronrotation becomes larger with increasing x, by
x-dpendence of the splitting of peak (2) shownby arrows. These results indicate that the local lattice distortion strongly correlates withthe broadening of MVE, i.e., Invar eﬀect.
References
1) K. Takenaka and H. Takagi :Appl. Phys. Lett. 87,
261902 (2005).
2) S. Iikubo et al. :Phys. Rev. B77, 020409(R) (2008).
3) S. Iikubo et al. : submitted to Phys. Rev. Lett.

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JAEA-Review 2011-050

1-1-60Existence of Ferroelectric Ice on Planets -a neutron studyH. Fukazawa
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195with the observed intensities drawn as dots.
It conﬁrms that ice XI is ferroelectric ice withaligned water molecules, as shown in Figure
1.
The particles of ice XI have long-range electric forces. The small ice XI of several micrometers in solar nebula may grow quickly
and attract electrons and ions. This special
character of ice XI becomes a key that solves
the mystery of the planet formation and thematerial evolution. Furthermore, a preliminary work using TAS-2 shows a clear diﬀerence in the spectroscopic data between ice XIand ice Ih. This implies that future telescopeand planetary exploration will ﬁnd huge ferroelectric ice and hydrogen-ordered ices in oursolar system.

Intensity (neutron counts)

The complex behavior of water and the unusual properties of hydrogen ordering in ferroelectric ice crystal continue to attract muchinterest. Whether ice in the space exists ashydrogen-ordered ices, is an important question. Some ordered ices have ferroelectricity,and long range electrostatic forces caused by
the ferroelectricity might be an important factor for planet formation.

Figure 1: The area (below the red line of 72 K) where
ice XI exists as a stable form in the solar system. Since
water molecules are aligned along c-axis (vertical direction), ice XI has ferroelectricity.

Recently, Fukazawa et al [1,2] imitatedthe ice of cold space and measured neutron
diﬀraction of the ice. The position of hydrogen became ordered at temperatures (below
76 K) of Uranus, Neptune and Pluto. H of thewater molecule has a positive charge. Basedon the neutron measurements, it is proposedthat ferroelectric ice, named ice XI, exists in
the Universe (Figure 1). Ice XI is the Hordered structure and KOH accelerates thephase transition process.
Figure 2 shows the diﬀraction pattern (dotted line) of NaOD-doped ice, which was kept
at 57 K for one day and kept at 68 K for 3
days. The solid lines, which are calculated
from the best-ﬁt model of the Rietveld reﬁnement with f = 0.27, are in good agreement
原子炉：JRR-3

装置：TAS-2(T2-4)

12000
8000
4000
0
20

40

60

80

2

100

120

140

(°)

Figure 2: Neutron diﬀraction pattern of 0.01-M
NaOD-doped ice at 68 K.

References
1) H. Fukazawa, et al. :“Astrophys. J. Lett.”, 652,
pp. L57-L60 (2006).
2) H. Fukazawa, et al. :“Physica B”, 385-386, pp.
113-115 (2006).
3) H. Fukazawa :“JAEA R&D Review”, p. 43 (2007).
4) H. Fukazawa :“Planetary People”, 16, pp. 7-12
(2007).
5) H. Fukazawa :“Hamon (The Japanese Society for
Nuetron Science)”, 18, pp. 97-102 (2007).

分野：中性子散乱（構造）㻙㻌 㻥㻞㻌㻙

JAEA-Review 2011-050

1-1-61
Nano-structure Analysis of ODS Ferritic Steels
for Fast Reactor Application
S. Ohtsuka1 , J. Suzuki2 , T. Kaito1 , S. Kim1 , M. Inoue1 , S. Obara1 and T. Asayama1
1Core and Structural Materials Group, Advanced Nuclear System R&D directorate
2
Neutron Optics Group, Quantum Beam Science Directorate

The oxide dispersion strengthened (ODS)
ferritic steel is a prospective material for fuelcladding tube of advanced fast breeder reactor(FBR). The most important task in the ODS
ferritic steel development is high-temperaturestrength improvement because the maximum
temperature of fuel cladding is designed to beas high as 973K for high thermal eﬃciency
and economical plant operation. In this research, nano-structure analysis of ODS ferritic steel was carried out using SANS-J-IIin JRR-3, and the correlation between nanostructure and high-temperature strength wasquantitatively evaluated with a view to obtaining insights into nano-structure control
technique for high-temperature strength improvement of ODS ferritic steel.
The ODS ferritic steel model alloys containing diﬀerent concentrations of excess oxygen(Ex.O) and Ti were prepared, where the basic chemical composition of JAEA ODS steel
for fast reactor application, i.e. 9mass%Cr0.13C-2W-0.35Y2 O3 , was adopted. Excess
oxygen is deﬁned as the value obtained bysubtracting O in Y2 O3 from the total O in
the steel. These steels were consolidated at
1423K (No.1, 3, 4) and 1473K (No.2), respectively. The size distribution and number density of nano-oxide particles were determinedfrom the measured SANS proﬁles, where lognormal size distribution was adopted. Figure 1 clearly displays that decreasing Ex.O
as well as increasing Ti provide for noticeable increase of nano-particle number density
and size reduction of nano-particles. Comparison of the proﬁles between No.1 and No.2
proves that the lower consolidation temperature is favored in terms of high population
nano-particle dispersion. The creep strengthof 9Cr-ODS steel was plotted against thesquare root of nano-particles number den原子炉：JRR-3

装置：SANS-J-IIsity in Fig.2, which shows the creep strengthof 9Cr-ODS steels is closely correlated withpopulation of nano-oxide particles.
Thesquare root of nano-particles number density
is known to be proportional to oxide dispersion strengthening. These results deﬁnitely
give the important knowledge that delicate
control of excess oxygen and titanium concentrations as well as appropriate choice ofconsolidation temperature are key points forhigh population nano-particle dispersion leading to drastic high-temperature strength improvement of ODS ferritic steel.

Figure 1: Size distribution of nano-scale oxide particles in 9Cr-ODS steels

Figure 2: Creep rupture strength versus square rootof nano-particle number densities.

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1.  ਛᕈሶᢔੂ 2 ⏛ ᕈ 


1. Neutron Scattering㻙㻌 㻥㻡㻌㻙

2 Magnetism

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JAEA-Review 2011-050

1-2-1

Neutron Inelastic Scattering of TbPd3S4
E. Matsuoka, K. Ohoyama(A), and H. Onodera
Department of Physics, Tohoku University, (A)Institute for Materials Research, Tohoku
University
The rare-earth (R) palladium bronzes
RPd3S4 crystallizes into a cubic NaPt3O4type crystal structure. R atoms form abody-centered cube and are subjected to a
cubic crystalline electric ﬁeld (CEF) represented by the cubic point group of Th [1].
Systematic studies along the R series haverevealed that the CEF ground states of 4f
electrons in RPd3S4 retain an orbital degeneracy [1].
In this system, DyPd3S4 with a quartet CEF ground state shows an antiferroquadrupolar (AFQ) ordering at 3.4 K [2].
However, the order parameter of the AFQ
phase has not been determined yet. For thedetermination of order parameter, we needto know the CEF scheme of 4f electrons.
The best experimental method for the estimation of CEF scheme is a neutron inelastic scattering. Unfortunately, it is difﬁcult toperform a neutron scattering of DyPd3S4
because of strong neutron absorption by
natural Dy nuclei. In this study, neutron inelastic scattering of TbPd3S4 has been performed and CEF scheme of TbPd3S4 has
been estimated. Our ﬁnal purpose is to estimate CEF scheme of DyPd3S4 by analogy
with that of TbPd3S4.
The temperature and Q dependence ofenergy spectra for the powder sample of
TbPd3S4 have been measured by the tripleaxis spectrometers HER (C1-1) and TOPAN(6G) with Ef = 3.6 and 14.7 meV, respectively.
The upper panel of Fig. 1 shows the energy spectra of TbPd3S4 at 7.2, 50 and 100
K for Q = 0.8 A-1 measured by HER. The
intensity of a shoulder-like anomaly at 0.25
meV decreases with increasing temperature. From the speciﬁc-heat measurement,
it has been expected that the ﬁrst excited
doublet or quartet is situated near ground
triplet [3]. It is therefore very probable thatthe anomaly at 0.25 meV corresponds tothe transition between the ground and theﬁrst excited states. The inset shows the energy spectra for Q = 0.8 A-1 above 1 meV.
Four peaks were observed at 2, 3.8, 4.7 and
5 meV. The lower panel of Fig. 1 showsthe energy spectra at 11, 104 and 300 K for
Q = 4 A-1 measured by TOPAN. Several
peaks and shoulder-like anomalies whose
intensities show temperature dependence
have been observed at energies indicatedby dashed lines in the ﬁgure.
The ground J-manifold of Tb3+ splits
into three triplet, one doublet and two singlets in cubic CEF. From the energy spectra obtained in this study, two possible CEF
schemes have been deduced for TbPd3S4,i.e., 0 - 0.25 - 5 - 9.5 - 18 - 21 meV or 0 - 0.25
- 3.8 - 11 - 21 - 29 meV.
References[1] K. Abe et al., Phys. Rev. Lett. 83 (1999)
5366.
[2] E. Matsuoka et al., J. Phys.: Condens.
Matter 13 (2001) 11009.
[3] E. Matsuoka et al., J. Magn. Magn.
Mater. 231 (2001) L23.

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JAEA-Review 2011-050

Fig. 1. Energy spectra of TbPd3S4 measured by HER(the upper panel) and TOPAN (the lower panel).
The data above 50 K are drawn with appropriate
offsets.

1-2-1

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JAEA-Review 2011-050

1-2-2

Spin Correlations of a Simple Cubic Antiferromagnet Pt3 Fe Alloy
R. Matsui, Y. Tsunoda
Waseda University
The ordered Pt3 Fe alloy has an
L12 (Cu3 Au)-type structure, in which
the corner sites are occupied by Fe and theface center sites by Pt, respectively. Since Pt
atoms carry no magnetic moments, Pt3 Fe
alloy is considered to be a simple cubic antiferromagnet. Below the Néel temperature(TN ∼ 180 K), Pt3 Fe alloy undergoes an
AF-AF phase transition at TS (TS ∼ 80 K).
At the high temperature phase, magnetic
structure is a (1/2 1/2 0)-type, but atthe low temperature phase, the (1/2 0 0)
Bragg peak coexists with decreasing of the(1/2 1/2 0) Bragg peak intensity.
Among simple cubic antiferromagnetic
structures, ferromagnetic and antiferromagnetic nearest neighbor spin couplings
coexist in both the (1/2 1/2 0)-type and(1/2 0 0)-type structures, suggesting existence of spin frustration. To study the spincorrelations of the simple cubic antiferromagnet, we carried out the neutron inelastic scattering experiments on a single crystal specimen of Pt3 Fe alloy in the paramagnetic phase. The measurements were performed at the T1-1 triple axis spectrometer,
JRR-3M.
Fig. 1 shows inelastic scattering intensity map obtained at 200 K (1.11 TN ) on
the (1 1 0) scattering plane (around the(1/2 1/2 1/2), (1/2 1/2 0) and (0 0 1/2)
RLPs) using the constant-E mode of operation at ΔE = 5 meV. Diffuse scattering peaks
were observed around (1/2 1/2 0) andthe (0 0 1/2) RLPs, which correspond tothe high temperature phase and low temperature phase, respectively, but no peakaround the (1/2 1/2 1/2) RLP. These data
indicate that the spin correlations of the(1/2 1/2 0)-type and the (1/2 0 0)-type
are competing in the paramagnetic phaseof T / TN = 1.11. We tried to reproduce
the intensity contour map of the (1 1 0)
plane using a simple classical Heisenberg

model under the random-phase approximation (RPA). To reproduce the observed
intensity map, we had to introduce up to
the 4th neighbor exchange coupling andthe exchange coupling parameters werecombined rather strict conditions. The ratio of the exchange parameters were determined as J1 : J2 : J3 : J4 = -1.0 : -0.90 : 0.25 : 0.10 (where the plus[minus] shows[anti]ferromagnetic coupling.)

Fig. 1. Inelastic scattering intensity map obtained onthe (1 1 0) scattering plane

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-2-3

Elastic Diﬀuse Scattering of Neutrons in Fe3 Pt Invar Alloys
M. Takasaka, Y. Tsunoda
Waseda University

The ordered Fe3 Pt alloy has an
L12 (Cu3 Au)-type structure, in which
the corner sites are occupied by Pt andface center sites by Fe, respectively. However, by thermal treatment, disordered
alloy is obtainable. Both ordered anddisordered Fe3 Pt alloys are ferromagnetic
and exhibit a small negative thermal
expansion below the Curie temperature(ordered:
TC =400∼500K, disordered:
TC =280∼380K), which is well known as
the Invar effect as well as Fe65 Ni35 alloy. A
martensitic phase transformation from fcc
to bcc structure occurs at low temperature.
Recently, by the neutron scattering measurement we performed, elastic diffuse
scattering with butterﬂy pattern was observed for typical Invar alloys Fe65 Ni35
around the (200) and (002) Bragg peak positions. Since diffuse scattering seems to bestrongly related with the Invar effect, we
tried to examine existence of diffuse scattering for another Invar alloy Fe3 Pt. Because Fe3 Pt alloy is unstable against themartensitic phase transformation at low
temperature, we used Fe72 Pt28 alloy in bothordered and disordered specimens. The
measurements were performed at the T11 triple axis spectrometer installed in thethermal guide of JRR-3M.
Fig. 1 shows elastic diffuse scattering intensity contour map for ordered Fe72 Pt28
alloy obtained at room temperature around(002). Diffuse scattering with butterﬂy pattern is clearly observed. In this ﬁgure,sharp ridge (the body of the butterﬂy) is
due to the mosaic spread of the sample.
The similar diffuse scattering with butterﬂy type is also observed for disordered
Fe72 Pt28 alloy. Diffuse scattering with butterﬂy type is a characteristic of the local lattice distortion. Since diffuse scattering withspecial pattern is common for three typical Invar alloys, Fe65 Ni35 , ordered and dis-ordered Fe3 Pt alloys, it is very likely that
this lattice distortion is related to the Invar effect. There are many things to examine such as temperature dependence, magnetic ﬁeld dependence, a difference by the
degree of atomic order etc. These are remained for future program.

Fig. 1. elastic diffuse scattering intensity contour
map for ordered Fe72 Pt28 alloy obtained at room
temperature around (002)

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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1-2-4
Magnetic structure of the n=3 frustrated square-lattice quantum spin system(CuCl)Ca2Ta3O10
H. Kageyama(A), Y. Tsujimoto(A), A. Kitada(A), T. Watanabe(A), Y. Ajiro(A), K.
Yoshimura(A), M. Nishi(B), K. Hirota(B)(A)Graduate School of Science, Kyoto University, (B)ISSP. University of Tokyo
A series of S=1/2 frustrated square-lattice
antiferromagnets (CuX)A2B3O10 (X=Cl,
Br; A=Ca, Sr, Ba, Pb; B=Ta, Nb) can be prepared by topotactic low-temperature ionexchange reactions using corresponding
triple-layered Dion-Jacobson type layered
perovskite oxides A’A2B3O10 (A’=Cs, Rb),
see Fig. 1. Quasi two-dimensional quantum magnetic properties could be expected
because nonmagnetic A2B3O10 perovskite
slabs act as a magnetically inert spacer, separating the magnetic CuX layer about 16 A.
We
recently
reported
that(CuBr)Sr2Nb3O10 has a 1/3 magnetization plateau in the magnetization curve
at low temperatures (Y. Tsujimoto et al.,J. Phys. Soc. Jpn. 76, 063711 (2007)). Thisis quite unusual since the 1/3 plateau isnormally expected in the triangule-basedlattices such as a triangular lattice andkagome lattice. In order to understandthe origin of the magnetization plateau in(CuBr)Sr2Nb3O10, we measured in 2006
the neutron diffraction of this material
at low temperatures at HERMES, but no
indication of magnetic order was obtained.

[100] . This spin structure is the same asthat found in the double-layered material(CuBr)LaNb2O7 and shows that the next
nearest neighbor Cu-Cu interactions are
dominant with respect to the nearest
neighbor interactions.

Fig. 1.
Crystal structures of A’A2B3O10 and(CuX)A2B3O10 before and after ion exchange reactions, respectively.

Therefore, as a next step, we measured the powder neutron diffractionof (CuCl)Ca2Ta3O10 which do not possess
any magnetization plateau. The powder
neutron diffraction patterns were obtained
at 2 K and 20 K, which is below and above
the temperature at which the temperaturedependence of the magnetic susceptibility shows the maximum. We found themagnetic order described as the propagation vector q = (pi, 0, pi), indicating
the so-called collinear magnetic ordering,where ferromagnetic chains along [010]
are antiferromagnetically coupled along
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JAEA-Review 2011-050

1-2-5

Neutron scattering study on (CuCl)LaTa2O7
H. Kageyama(A), A. Kitada(A), Y. Tsujimoto(A), Y. Ajiro(A), K. Yoshimura(A), M.
Nishi(B), N. Matsuura(B), K. Hirota(B)(A)Graduate School of Science, Kyoto University, (B)ISSP. University of Tokyo
Spin-structure of the square-lattice antiferromagnet is trivial as long as the nearest
neighbor interactions are considered. However, inclusion of antiferromagnetic next
nearest neighbor interactions induces frustration, leading to non-trivial phases suchas spin-liquid state.
We demonstrated from magnetic susceptibility and neutron scattering experiments that (CuCl)LaNb2O7, preparedby topotacic ion-exchange reaction of
RbLaNb2O7 with CuCl2, does not show
any sign of long range magnetic ordering
at low temperatures, indicating spindisordered ground state [1].Here, the S= 1/2 square lattices are formed by the
Cu-Cl layers, which are separated by thenonmagnetic LaNb2O7 perovskite blocks.
In contrast, the isostructural compound(CuBr)LaNb2O7 exhibits the long range
magnetic order at 32 K. The neutron powder diffraction study at HERMES and 5G
gave the spin structure of this material, acollinear type of order with a modulation
vector of (pi, 0, pi). Such a spin structure is
expected when the next nearest neighborinteraction dominates over the nearest
neighbor one.The difference in the groundstate between the Cl and Br compounds
could be explained in terms of the difference in superexchange interactions
between Cu-Cl-Cl and Cu-Br-Cu.

(CuBr)LaNb2O7.This could not be explained by the abovementioned scenario.
This observation indicates that the superexchange path via TaO6/NbO6 also
contribute to the magnetism.
[1] H. Kageyama et al., J. Phys. Soc. Jpn. 74,
1702 (2005)[2] N. Oba et al., J. Phys. Soc. Jpn. 75,
1133601 (2006)

Fig. 1. Temperature dependence of the (1/2, 0, 1/2)
magnetic reﬂection for (CuCl)LaTa2O7

Under the proposal number 7535, wehave performed the neutron inelastic andelastic scattering study on (CuCl)LaTa2O7,
again isostructural of (CuCl)LaNb2O7.
Sicne pentavalent Ta and Nb have nearly
the same ionic radii, the two compounds
have nearly same lattice parameters.
However, (CuCl)LaTa2O7 show themagnetic ordering of the same type of
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JAEA-Review 2011-050

1-2-6Electric polarization induced by a proper helical magnetic ordering in a delafossite
multiferroic CuFe1−x Alx O2
T. Nakajima, S. Mitsuda, S. Kanetsuki, K. Tanaka, T. Fujii, N. Terada1 ,M. Soda2 , M. Matsuura2 , K. Hirota2 .
Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601, Japan
1 ICYS, National Institute for Materials Science, Ibaraki 305-0044, Japan
2 Institute for Solid State Physics, University of Tokyo, Kashiwa 277-8581, Japanence between ION and IOFF for both of +q
and the −q magnetic satellites reﬂections(see Fig.1(b)). After cooling the sample under a poling electric ﬁeld (120 kV/m) parallel to the helical axis, ION was greater than
IOFF for the +q reﬂection, and this relationship between ION and IOFF was reversed
for the −q reﬂection, as shown in Figs. 1(d1) and 1(d-2). These results clearly demonstrate that proper helical magnetic orderingin CuFe1− x Alx O2 generates a spontaneouselectric polarization along the helical axis,
and there is one-to-one correspondence between the polarity of local polarization vector and the spin helicity, as illustrated inFig. 1(a).
References[1] T. Nakajima et al.: JPSJ 76 (2007)043709.
[2] H. Katsura et al.: PRL 95 (2005)057205.
Right-Handed-HelicalP(b)

C(=Si Si+1)

(00L)

(a)

(HH0)

(003)

[001]

i

[110]
[110]

i+1

P

Left-Handed-Helical

L=

3
2

~32

C

counts/20 sec

1000

H= 1
2

(000)

i+1

i

-q

+q

1

1

( 2 -q, 2 -q, 32 )(q, q, 32 )(c-1) E [110] = 128[kV/m]

1000(c-2) E [110] = 128[kV/m]

750

IOFF
ION

500

250

250
0

0

(d-1) E [110] = 120[kV/m](d-2) E [110] = 120[kV/m]

750

750

500

500

250

250

0
0.19

0.2

0.21

0.22

H [r. l. u.]

0.23

0.28

0.29

0.3

0.31

counts/60 sec

counts/20 sec

750

500

counts/60 sec

Delafossite CuFe1− x Alx O2 has been thesubject of intense recent interest, becauseof the ferroelectricity accompanied by aproper helical magnetic ordering[1]. The
local spin-polarization coupling in this system cannot be explained by the ‘spincurrent model’ proposed by Katsura etal.[2], which successfully explains the ferroelectricity in cycloidal magnetic orderings of certain transition metal oxides such
as TbMnO3 . Hence, we performed polarized neutron diffraction measurements
on CuFe1− x Alx O2 (x = 0.02) with applied
electric ﬁeld at the triple-axis neutron spectrometer PONTA installed at JRR-3, in order to identify the local spin-polarization
coupling in this system.
A single crystal of CuFe1− x Alx O2 withx = 0.02 of nominal composition was
prepared by the ﬂoating zone technique.
An incident polarized neutron with energy
34.05 meV was obtained by a Heusller (111)
monochromator. The ﬂipping ratio of thepolarized neutron beam was ∼ 19, and thepolarization vector of the incident neutron,pN , was set to be parallel or antiparallel tothe scattering vector, κ, by a guide-ﬁeld of ahelmholtz coil and a spin ﬂipper. The collimation was 40 -40 -40 -40 . The sample wasmounted in a pumped 4 He cryostat with ahexagonal (hhl) scattering plane.
Typical diffraction proﬁles of magnetic
reﬂections in the ferroelectric phase (T = 2K) are shown in Figs. 1(c-1)-(d-2), in which
ION and IOFF denote the intensities measured when pN  −κ and pN  κ, respectively. As shown in Figs.1(c-1) and 1(c2), after cooling the sample under a poling electric ﬁeld (128 kV/m) perpendicular to the helical axis, there was no differ-

00.32

H [r. l. u.]

Fig. 1. (a)The relationship between spin arrangements and polarization vectors. (b)The location of
the magnetic reﬂections. [(c-1)-(d-2)] The diffraction
proﬁles at T = 2K.

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JAEA-Review 2011-050

1-2-7Electric ﬁeld dependence of magnetic ordering of a delafossite multiferroic
CuFe1−x Alx O2
T. Nakajima1 , S. Mitsuda1 , H. Kimura2 , and Y. Noda2
1 Department of Physics, Faculty of science, Tokyo University of Science 1-3 kagurazaka,

shinjuku-ku, Tokyo, 162-8601

2 Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai

980-8577
application of a poling electric ﬁeld within| E| <∼ 2200 kV/m does not affect the fractions of the three magnetic domains, implying that the fractions of the three magnetic
domains are determined by the lattice distortion, which have been already occurredin the high-temperature (paraelectric) partially disordered phase [2].
However, we found that the diffraction
proﬁles of the magnetic reﬂections in the
ferroelectric phase are sharpened by applying the poling electric ﬁeld, as shownin Fig. 1(c), suggesting that an application of the poling electric ﬁeld improves
the magnetic correlation in the ferroelectric phase. For the quantitative evaluationof the changes in magnetic correlation, further investigations are awaited.
References[1] T. Nakajima et al.: PRB (in press).
[2] N. Terada et al.: JPSJ 75 (2006)113702.
Integrated Intensity [arb. units](a) 150(b)

E [110](-2q,q,0)100

b*(q,q,0)50(q,q,3/2)-domaina*(-2q,q,3/2)-domain(q,-2q,0)(q,-2q,3/2)-domain
0

0

500

1000

1500

2000

c*

2500

Poling E-field [kV/m](c)counts / 20sec

Delafossite CuFe1− x Alx O2 has been ofincreasing interest as a new class of multiferroics, because of the ferroelectricity accompanied by a proper helical magnetic ordering. Recent polarized neutron diffraction measurements on CuFe1− x Alx O2 withx = 0.02 under applied electric ﬁelds up
to 160kV/m revealed the correspondence
between the magnetic propagation wave
vector and the local electric polarization
vector[1]: speciﬁcally, the direction of thelocal electric polarization vector is parallel(or antiparallel) to the magnetic modulation wave vector projected in the hexagonal[001]-plane. Since this system has the threemagnetic domains reﬂecting the three-foldsymmetry of the crystal structure (see Fig.
1(b)), it is natural to anticipate that the poling electric ﬁeld should favor the wave vector for which the electric polarization canbe maximized. However, no signiﬁcantchanges are detected in the magnetic domain distribution under the electric ﬁeld
within E < 160kV/m applied along the[110] axis[1].
In present experiments, we have investigated the magnetic domain distributions
in CuFe1− x Alx O2 (x = 0.02) under electric ﬁelds up to 2200kV/m along [110]axis, using the four-circle neutron diffractometer FONDER(T2-2) installed at JRR-3.
The wavelength of the incident neutron is
1.24Å. The closed-cycle He-gas refrigerator
was used to provide access to the temperature down to 2.5K.
Fig. 1(a) shows the poling electric ﬁeld
dependence of the integrated intensities of
the three equivalent magnetic reﬂections,which are proportional to the fractions of
the magnetic domains. This shows that the800

T=2.5K
600

cooled with E-field 1911kV/mcooled without E-field

400
200
0
0.18

0.2

0.22

0.24

0.26

0.28

0.3

0.32

h [r. l. u.]

Fig. 1. (a) The poling E-ﬁeld dependence of theintensities of the three equivalent magnetic reﬂections. (b) [001]-projection of the three equivalent
propagation wave vectors. (c) Typical diffraction
proﬁles in the ferroelectric phase.

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JAEA-Review 2011-050

1-2-8
Eﬀective random-ﬁeld domain-state in a diluted frustrated magnet CuFe1−x Alx O2
T. Nakajima, S. Mitsuda, H. Honma, H. Tsuchida
Department of Physics, Faculty of science, Tokyo University of Science 1-3 kagurazaka,
shinjuku-ku, Tokyo, 162-8601
Fig. 1(d)). In particular, the existence ofa Lorentzian-squared term indicates thatthe system breaks into a large number ofsmall magnetic domains. We found thatthe width of the S(q), κ, increases withincreasing Al3+ -concentration x (see Fig.
1(c)). This indicates that the average size ofmagnetic domains decreases with increasing x. We also found the contribution of
the Lorentzian term in S(q) increases withincreasing x, as shown in Fig. 1(c). Thisimplies that the system gradually changes
from a random-ﬁeld domain state to a spinglass like disordered state, as the substitution increases. The further detailed analysis is now in progress.
References[1] J. van Duijn et al.: PRL 92 (2004)077202.
[2] T. Nakajima et al.: JPCM 19(2007)145216.
(b) x=0.20 (T=2.0K)
104

1000

1000

counts/20sec

counts/20sec(a) x=0.15 (T=2.0K)
104

100

10

0.12

0.16

0.2

0.24

0.28

0.1

κ

ab

[r. l. u.]

(c)
0.8

0.003

0.6

0.002

0.4

0.001

0.2

0.1

0.15

0.2

0.15

0.2

0.25

0.3

H [r. l. u.]

1

0.004

0
0.05

100

10

H [r. l. u.]
0.005

Ratio of Lsq and Lrz Amplitude (B/A)

Geometrically frustrated spin systems
have been extensively investigated, because they exhibit a variety of exotic
magnetic orderings, which spans from acomplex noncollinear magnetic state to aspin-glass like disordered state. One of
the unusual magnetic state in this system is the Partially-Disordered (PD) state,in which magnetically disordered sublattices exist.
Recent studies on diluted
triangular lattice antiferromangets suchas CsCo1− x Mgx Br3 [1] and CuFe1− x Alx O2( x = 0.10)[2], which exhibit the PD magnetic orderings, revealed that a combination of the PD magnetic ordering and siterandom magnetic vacancies can generate
effective random-ﬁeld even in the absenceof external magnetic ﬁeld.
For the systematic study on this effective random-ﬁeld effect in the diluted frustrated magnet, we performed
neutron diffraction measurements on
CuFe1− x Alx O2 samples with x = 0.15
and 0.20, using the triple-axis neutron
spectrometer HQR(T1-1) installed at JRR-3.
The collimation open-’40-’40-’40 was employed. The wavelength of the incident
neutron is 2.44Å. The single crystal of
CuFe1− x Alx O2 samples were mounted ina 4 He-pumped cryostat with a hexagonal(hhl )-scattering plane. In order to evaluate
the magnetic correlation length quantitatively, we analyzed the scattering proﬁle,using Multi-Proﬁle-Deconvolution method
presented in Ref. [2].
Figs. 1(a) and (b) show the scattering
proﬁles of the x = 0.15 and 0.20 sample at T = 2K and the results of MPDanalysis for these proﬁles. For both samples, the scattering function of the magnetic reﬂections are well described by thesum of a Lorentzian term and a Lorentziansquared term with anisotropic width (see(d) Scattering Function
S(q) =+

A
2(1+ (qa2 +qb2 )/Kab+qc2 /Kc2 ) 2
B
2
1+ (qa2 +qb2 )/Kab+qc2/Kc2

00.25

Al concentration x

Fig. 1. Typical scattering proﬁles of (a) x = 0.15 and(b) x = 0.20 samples at T = 2.0K. (c) x dependenceof the width of S(q) and the ratio of amplitude of
Lrz and Lsq term at T = 2K. The data of x = 0.10 istaken from Ref. [2] (d) Deﬁnition of the S(q).

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JAEA-Review 2011-050

1-2-9
Polarization analysis neutron scattering study of magnetic correlations in randommagnet Fe65(Ni-Mn)35
K. Motoya and Y. Muro
Department of Physics, Faculty of Science and Technology, Tokyo University of Science
A previous neutron scattering study
showed that the short-range ferromagnetic
and antiferromagnetic correlations coexist in wide concentration and temperature ranges of a random magnet system
Fe65(Ni-Mn)35 [1]. Magnetic ﬁeld variations of diffuse scattering patterns arising from these ferromagnetic and antiferromagnetic correlations have shown that theregions of these two kinds of correlations
coexist separately in this system [2]. In thisreport, we present the result of polarization
analysis experiment of this system.
The magnetic diffuse scattering patterns arising from ferromagnetic correlations (ferromagnetic clusters) observed
around (111) Bragg point are well traced bya Lorentzian (LOR) function. Figure 1 (A)and (B) show the magnetic ﬁeld variationsof the amplitude (AL) and the width (κ L)of the spin-ﬂip and non-spin-ﬂip components, respectively. The result shows thatthe number and the average size of ferromagnetic clusters decrease with increasingﬁeld. This seems to be inconsistent with themagnetization behavior. We have made a
scenario of magnetic ﬁeld variation of ferromagnetic clusters consistent with the results of the neutron scattering and magnetization measurements [2].
The diffuse scattering signals arisingfrom antiferromagnetic correlations (antiferromagnetic clusters) have been measured around (100) and (110) Bragg points.
These patterns are well traced by a LOR
function. The ﬁeld variations of the amplitude and the width of the spin-ﬂip andnon-spin-ﬂip components are shown in
Fig.1 (C) and (D), respectively.

Based on the unpolarized [2] and thepresent polarization analysis measurements, we will determine the magnetic
ﬁeld variations of the number, size and orientation of the ferromagnetic clusters aswell as the magnetic structure of the antiferromagnetic clusters.
[1] K. Motoya and K. Hioki, J. Phys. Soc.
Jpn. 72 (2003) 930.
[2] K. Motoya et al., Phys. Stat. Sol. (submitted)

Fig. 1. Magnetic ﬁeld variations of the amplitude
and the width of the scattering patterns arising fromferromagnetic and antiferromagnetic clusters.

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JAEA-Review 2011-050

1-2-10Magnetic excitations in the random-exchange Ising system (Fe-Zn)F2 near the
percolation threshold
K. Motoya, Y. Muro, N. Aso (a) and D. P. Belanger (b)Tokyo University of Science, (a) ISSP, (b) University of California, Santa Cruz
The diluted antiferromagnet (FexZn1-x)F2
has been extensively studied in the past
as an ideal system for the studies ofthree-dimensional random-exchange Isingmodel. Previous neutron scattering studies
of magnetic excitations of this system haverevealed the following [1, 2]. For x=0.59 thespin-wave-like energy spectrum observed
near q=0 changes to a form of localized
excitations as q increases. The overall energy width and position of the spectrum atthe zone boundary can be described by the
local mean ﬁeld (LMF) model. The spectrum from x=0.40 at q=0 consists of four
evenly spaced excitation peaks. However,
the overall structure is higher in energy
than the predicted excitations of the LMF
theory.
In order to clarify the total propertyof magnetic excitations of this system including the percolation threshold region(xp=0.24), we made high-energy-resolution
inelastic neutron scattering measurements.
Two single crystals of x=0.25 (total weight 4.1g) were aligned with the caxis vertical to the horizontal scattering
plane. Measurements were performed using a horizontally-focusing analyzer on
C1-1 spectrometer. The energy resolution
varies from 0.08meV (FWHM) to 0.17meVas the energy transfer increases from 0 to
7meV with the ﬁnal neutron energy ﬁxed
at Ef=3.1meV.
Figure 1 shows inelastic scattering intensity vs energy for x=0.25 measured at
T=0.7K and various value of q. For all q
values (from the zone center to the zone
boundary) well resolved 6 peaks were observed. The position of each peak does not
move with increasing q.

These features strongly suggest that theobserved spectrum is attributed to the excitations of individual spins with various local environment. The bottom panel of Fig.1
shows the excitation spectrum of individual spins based on the LMF theory.
At T=10K no appreciable change wasobserved in the spectra. As increasing temperature the peaks gradually broaden andﬁnally fade into a broad spectrum.
This shows that the system ”freezes” below
T=10K.
[1] C. Paduani et al., Phys. Rev. B 50 (1994)
193.
[2] Y. W. Rodriguez et al., J. Mag. Mag.
Mater. 310 (2007) 1546.

Fig. 1. The scattering intensity vs energy at T=0.7K
measured at various q. The bottom panel is the LMF
prediction.

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JAEA-Review 2011-050

1-2-11
Inelastic Neutron Scattering Study on Triangular Lattice Antiferromagnet CuFeO2
T. Nozaki, K. Hayashi, and T. Kajitani
Department of Applied Physics, Graduate School of Engineering, Tohoku University, Sendai,
980-8579
reason of its broadning is the creation ofmagnon branches.[3, 4] As the temperature
increases, the peak position moves closer tothe central peak, i.e. the frequency of themagnon mode becomes lower. This temperature dependence is conceivably due tothe spin-wave interactions.[5] It should be
noted that a broad magnetic critical scattering component appears in the spectra taken
at 12.5 K and 16 K.
References[1] N. Terada et al.: Phys. Rev. B 74 (2006)
180404, and references therein.
[2] K. Hayashi et al.: Jpn. J. Appl. Phys. 46(2007) 5226.
[3] N. Terada et al.: J. Phys.: Condens. Matter
19 (2007) 145241.
[4] F. Ye et al.: Phys. Rev. Lett. 99 (2007)
157201.
[5] T. Oguchi: Phys. Rev. 117 (1960) 117.

16 K

S (ω )

Geometrically frustrated magnetic systems have received considerable attention in recent years due to the presence of extraordinary magnetic properties. As a model material of the magnetically frustrated triangular lattice antiferromagnet, CuFeO2 shows successive magnetic phase transitions from an Ising-like 4sublattice phase (↑↑↓↓) to a paramagnetic
phase through a partially disordered phase(TN2 ∼ 10.5 K < T < TN1 ∼ 14.0 K).[1] To
understand these complicated magnetic orderings, it is needed to elucidate magnons
and phonons in the CuFeO2 system in thewide temperature range. In this study, wemeasure inelastic neutron scattering spectra of powder CuFeO2 below and over TN1
and TN2 .
Inelastic neutron scattering measurements were carried out by the use of a cold
neutron spectrometer, AGNES. A wave
length of the incident neutron was 4.22
Å. The energy value of the scattered neutron was determined by the time-of-ﬂight
method. The energy resolution was about
0.1 meV in the present experimental condition. The data acquisition time was about
20 h. Powder CuFeO2 sample was synthesized by the solid state reaction method as
described elsewhere.[2]Figure 1 shows inelastic neutron scattering intensitiy, S(ω ), of the CuFeO2 powder taken at 7.5, 10, 11, 12.5, and 16 K,
where ω is the angular frequency. The
horizontal axis is the energy transfer values of the incidence. The negative sideof the spectra corresponds to the energy
loss side, i.e. the Stokes side. The central
peaks at 0 meV are the elastic scattering
components. There is a large and broad
peak around −2 meV in each spectrum below 12.5 K, corresponding to the creationof locarized magnon mode. One possible

12.5 K

11 K

10 K

7.5 K

-3
-2
-1
0
Transfer energy ( meV )Fig. 1.
Inelastic neutron scattering spectra of
CuFeO2 powder at 7.5, 10, 11, 12.5, and 16 K.

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JAEA-Review 2011-050

1-2-12
Search for magnetic reﬂections in a heavy fermion antiferromagnet CeTe3
N. Aso, K. DeguchiA , G. F. ChenA , N. K. SatoA , H. Yoshizawa
NSL-ISSP, Univ. of Tokyo, Graduate School of Sci., Nagoya Univ.A
References[1] V. Brouet et al., Phys. Rev. Lett. 93, 126405(2004).
[2] H. Komoda et al., Phys. Rev. B 70, 195101(2004).
[3] Y. Iyeiri et al., Phys. Rev. B 67, 144417(2003).
[4] G.F. Chen et al., in preparation.
[5] TAIYO NIPPON SANSO CORPORATION. Tokyo 142-8558, Japan.
2

060

1000
9
8

040

7
6
5

(a)

151
081

3

170

080
111
131

4

150

Intensity (cnts/M800k)

CeTe3, T=0.75K

2Int.(T=0.75K)-Int.(T=5K)

300

Int.(T=2K)-Int.(T=5K)

CeTe3 belongs to the family of quasi-two
dimensional charge-density-wave (CDW)
compounds RTe3 (where R = Y, La-Sm, GdTm). [1, 2] The crystal structure is weakly
orthorhombic with the lattice parameters ofa ≈ c ∼ 4 Åand b ∼ 25 Å. In low temperature regin, there has been reported somemagnetic ordering below T ∼ 3K from thesusceptibility measurements. [3] Very recently, Chen et al. found that CeTe3 exhibits another (possibly) magnetic ordering
below T ∼ 1.2 K by the speciﬁc heat andsusceptibility measurements. [4] From thesusceptibility measurements, the phase below at T ∼ 1.2 K seem to the 2nd-order antiferromagnetic ordering.
In this context, the main goal of this work
is to determine the order parameters of
the low-temperature two phases by neutron diffraction technique. Powder sample
of m ∼ 10 gram were prepare and put in aaluminum can ﬁlled with a He gas. It wascooled down to 0.75 K using a 3 He cryostat. [5] Neutron diffraction experiments
were performed at PONTA and HQR in the
research reactor JRR-3.
Figure 1 (a) shows powder pattern of
CeTe3 obtained at HQR with the incident
energy Ei ∼ 13.5 meV and the other conﬁgurations of G-Open-PGF-40’. Although
one can clearly see some strong Nuclear
Bragg peaks denoted by the indices in theﬁgure, no distinct magnetic Bragg peak areobserved. Thus we tried to subtract the
scattering in the paramagnetic state of T =5 K as the background one. Figure 1 (b)and (c) correspond to the scattering at T =0.75 K and T = 3 K, respectively. One canclearly see no distinct magnetic Bragg peakin the both two phases. The possible reason is that the magnetic moment of the twophases is very small less than 0.3 μB /Ce.
We now try to go to the single crystalline
studies in the next.

(b)

200
100
0
-100
-200
-300
300

(c)

200
100
0
-100
-200
-300
0

10

20

30

40

50

60

A2 (degree)

Fig. 1. (a) Powder pattern of CeTe3 obtained at T
= 0.75 K. (b) Subtracted proﬁle at 0.75 K. Small deviation at small angles perhaps comes from the Hegas scattering in the aluminum cell. (c) Subtracted
proﬁles at 2 K.

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JAEA-Review 2011-050

1-2-13Magnetic structure of TbCoSn
M.Kurisu, A.Tada, G.Nakamoto, T.Tsutaoka(1) and Y.Andoh(2)Japan Advanced Institute of Science and Technology, Ishikawa 923-1292, Japan(1)Graduate School of Education, Hiroshima University, Hiroshima 739-8524, Japan(2)Faculty of Regional Sciences, Tottori University, Tottori 680-8551, Japan
RTX (R: rare earths, T: transition metals, X: metalloids) compounds crystallize
in the epsilon-TiNiSi-type orthorhombic
structure. Their magnetic property is characterized by
1. relatively lower antiferromagnetic ordering temperature TN below 20 K,
2. highest TN not at R=Gd but at Tb,
3. multi-step metamagnetic transitions in
the ordered state along the easy axis ofmagnetization,
4. incommensurate magnetic structures inthe series.[1]Recently, it has been revealed that RRhGe(R=Tb and Dy) compounds also possess
successive magnetic transitions below the
Neel temperature from the magnetic andspeciﬁc heat measurements. Our interest isin the role of crystalline electric ﬁeld (CEF)
effect and determination of magnetic structures in the series. In the present report, weshow preliminary experimental results on
TbCoSn.

ceptibilities is well accounted for the threeprincipal axes by the CEF calculation basedon the point charge model. It is noted thatthe easy axis of magnetization is the a-axis
in TbCoSn while it is the b-axis for otherisostructural TbTX compounds. The sign ofsecond order CEF parameter appears to bea dominant factor to determine the magnetic anisotropy.
The variation of magnetic reﬂection at(0 0.25 0) with temperature is displayed in
Fig.1. This also supports the existense of
low temperature phase below 4 K. A further data acquisition is needed to determine the magnetic structure of the compound.
References[1] Y.Andoh, M.Kurisu, and S.Kawano,
Journal of Magnetism and Magnetic Materials, 177-181 (1998) pp.1063-1064.

Single-crystalline TbCoSn ingots weregrown by a Czochralski method using a tetra-arc furnace in puriﬁed Ar
atmosphere. The magnetic and speciﬁcheat measurements were performed by a
SQUID magnetometer and a PPMS, respectively. The neutron diffraction measurements were performed at T1-1:HQR spectrometer installed at JRR-3M.

100000

1.8 K
8.8 K
22 K

I (counts/30 sec)

TbCoSn
80000
60000
40000
20000
0
-0.10

The magnetic susceptibility shows that
antiferromagnetic ordering takes place at
20.2 K. Below TN, an anomaly indicative ofanother magnetic transition is observed at
4 K for the three principal axes. The speciﬁcheat measurement also indicates the twomagnetic phases down to 1.8 K. The temperature dependence of the magnetic sus-

-0.05

0.00

0.05

l in (0 0.25 l )0.10

Fig. 1. Magnetic reﬂection at (0 0.25 0).

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JAEA-Review 2011-050

1-2-14Pressure induced incommensurate–commensurate magnetic phase transition in
multiferroic HoMn2 O5
H. Kimura1 , K. Nishihata1 , Y. Noda1 , N. Aso2 , T. Fujiwara3 and Y. Uwatoko2
1 IMRAM, Tohoku University
2 ISSP, The university of Tokyo
3 Department of Physics, Yamaguchi University
RMn2 O5 is well known as “multiferroics”
where the ferroelectric and antiferromagnetic order coexist and their order parameters couple with each other. This systemessentially involves geometrical magnetic
frustration, which leads to the long-period
magnetic order and the complex magnetic
phase diagram as a function of temperature. It was found that in HoMn2 O5 ,magnetic-ﬁeld-induced incommensurate–commensurate magnetic phase transition
occurs in which the ferroelectic state areconcomitantly induced[1]. This result indicates that the external ﬁeld can control thedielectric phase through the control of competing magnetic ground states. Recently,
it was found that the ferroelectric phaseis induced by applying a hydrostatic pressure in HoMn2 O5 [2], indicating that thecommensurate magnetic phase might appear by applying pressure. In the present
study we thus performed neutron diffraction measurements under hydrostatic pressure to search the pressure induced magnetic phase transition in HoMn2 O5 .
Single crystal of HoMn2 O5 was inserted
in Cu-Be clamp cell and the pressure wasapplied up to 1.25 GPa. The measurement of magnetic peaks was performed using the triple-axis spectrometer AKANE installed at T1−2 thermal guide in JRR-3M.
At 0 GPa, shown in Fig. 1 (a), a pair ofmagnetic peaks locate around (0.5±0.02 0
1.73), indicating that the magnetic order isincommensurate. Upon applied pressure,shown in Fig. 1 (b), there is a strong peak at
the commensurate position (0.5 0 1.75) witha minor incommensurate peak, showingthat the commensurate phase is induced.
We mapped out the pressure–temperaturephase diagram for the magnetic orderedphases, showing the one-to-one correspondence with that for the dielectric phases[2].
References[1] H. Kimura et al.: JPSJ 75 (2006) 113701.
[2] C. R. Cruz et al.: PRB 76 (2007) 174106.

Fig. 1. Contour maps in ( H 0 L) zone of magnetic
Bragg reﬂection under (a) 0 GPa and (b) 1.25 GPa,taken at 6 K.

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Defect-induced short-range magnetic order in Co2(OD)3Cl
X.G. Zheng, M. Hagihala, T. Yamashita
Faculty of Science and Engineering, Saga University, Saga 850-8502, Japan
In recent years we found a new geometric frustration system Cu2(OH)3Cl andCo2(OH)3Cl with a 3-dimensional network of corner-sharing tetrahedrons of the
Cu2+ and Co2+ spins, respectively 1-3.
We found coexisting antiferromagnetic order and spin ﬂuctuation down to T=0 in
ideal quantum spin material Cu2(OH)3Cl
2, and a kagome-ice-like partial ferromagnetic order in Co2(OH)3Cl 3, which raise
great interest on this new material system. The latter compound can be comparedwith the rare-earth pyrochlore compounds
Ho2Ti2O7, Dy2Ti2O7 and Ho2Sn2O7, i.e.,the spin ice compounds. In these materials the spin alignment and the macroscopic quantum degeneracy are shown to
be a magnetic equivalence of the ice rule inwater ice. The spin ice has received intense
attention because of the dynamics associated with the macroscopic degeneracy areexperimentally accessible by many magnetic probes, and because the geometricalfrustration of competing interactions is an
essential element of important problems
in ﬁelds extending to protein folding andneural networks. The experimentally observed degeneracy and zero-point residual
entropy for water ice and spin ice apparently contradict a fundamental principle ofthermodynamics (the 3rd law), which demands a single ordered ground state andhence zero entropy. As to the spin ice, aﬁrst-order phase transition to a true groundstate is theoretically predicted, but has notbeen observed to date, despite rigorous efforts down to the experimentally attainabletemperature of 10 mK. Whether the spin ice
keeps the macroscopic quantum degeneracy down to 0 K remains an open and controversial issue.
Because Co2(OH)3Cl has a comparatively very higher transition temperatureof TC = 10.5 K, we explored the possibil-

ity of a low-temperature order with impurity doping. For this purpose neutron
diffraction experiment was carried out at
T1-3 (Hermes) using powder sample of(Co0.9Al0.1)2(OD)3Cl.
Figure 1 shows the neutron diffraction patterns for (Co0.9Al0.1)2(OD)3Cl at typicaltemperatures. The results clearly show thata short-range spin correlation develops below around 4 K. AC and DC susceptibility
measurements suggest that the remaining
spin degree of freedom freeze completely
below 4 K with a drastically increasing relaxation time.
The above-described result can be considered as an interesting analogy to the
low-temperature anomaly in doped water
ice, especially in the light of its relevanceto the problem of residual entropy in icewater or spin-ice transition. We hope it
contributes to a complete understanding of
the true ground state of geometrically frustrated systems.
References
1. X.G. Zheng et al., Phys. Rev. B 71, 052409(2005).
2. X.G. Zheng et al., Phys. Rev. Lett. 95,
057201 (2005).
3. X.G. Zheng et al., Phys. Rev. Lett. 97,
247204 (2006).
4. X.G. Zheng et al., Phys. Rev. B, in press.

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Fig. 1.
Neutron(Co0.9Al0.1)2(OD)3Cl.

diffraction

resultfor

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1-2-16

Inelastic neutron scattering on DyB4
Takeshi Matsumura, Daisuke Okuyama, and Takuya Mouri
Tohoku University

DyB4, belonging to a space group
P4/mbm, has been attracting interest as asystem where the quadrupolar and magnetic degrees of freedom exhibit anomalous correlations on the so-called ShastrySutherland lattice of Dy atoms. DyB4 exhibits two phase transitions at TN1=20.3 K
and at TN2=12.7 K. It has already been established that the c-axis component of themagnetic moment orders antiferromagnetically below TN1, whereas the c-plane componet somehow remains paramagnetic until TN2 by magnetic susceptibility and elastic constant measurements. However, resonant x-ray diffraction and neutron diffraction experiments on single crystalline samples performed by us show short-rangedordering of the c-plane magnetic component between TN2 and TN2, indicating thatthe time scale of the ﬂuctuation is much
longer than 10ˆ(-12) sec, the time scale ofneutron diffraction, but shorter than 10ˆ(7) sec, the time scale of ultrasonic measurement. Therefore, in order to investigate
the difference in the magnetic states in thethree phases, we have performed inelastic
neutron scattering experiment on DyB4.
Inelastic neutron diffraction on DyB4 isvery difﬁcult because the absorption by
natural Dy is quite large (˜970 barn), eventhough we used enriched 11-Boron isotope
to prevent absorption by 10-Boron. Then,
we sliced the single crystal samples into
the plates with thicknesses of 0.5 mm, maximizing the scattered neutrons. We prepared four sliced samples and orientatedthem within an error of 0.5 degree We performed constant-Q scans at positions closeto (1, 0, 0), (2, 0, 0), (1, 0, 0.5), (1, 0, 1), (1, 0,2), and (0, 0, 1) at three temperatures at 25
K, 15 K, and 4.0 K.
Figure shows the inelastic spectra at (1.05,
0, 0). At 25 K, we clearly observe two excitations at 4.5 meV and 6.5 meV. They are con-sidered as the crystal ﬁeld excitations since
they are also observed at other Q-positons.
In addition, we observe a low energy excitation below 2 meV. Fitting of the spectrum
indicates that the excitation is at 1.4 meV.
At 15 K in the intermediate phase, the energies of the higher enegy excitations shift
to higher energies, while the low energy
excitations remain unchanged. Below TN2,
at 4 K, the low energy excitation vanishes
and shifts to the well resolved excitation at
2.5 meV. This behavior is the same as thatof HoB4. The high energy excitations also
move to higher energies.
The change in the excitation spectraat three temperatures in the three phasesshows that the magnetic state is obviously
different. Phase I above TN1 is paramagnetic. In phase II between TN1 and TN2,
the c-axis component is ordered. The cplane component is also ordered in a shortrange, but it is not static. If it is static, thespectrum should have the same characteristic as in phase III below TN2, which is not
the case.
To summarize, we have suceeded in measuring the inelastic excitation spectra on
DyB4 with high absorption by Dy. Thechange in the spectrum for the three magnetic phases has been clearly observed.

Fig. 1.

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Neutron diﬀraction in magnetic frustration systems with a 40T pulsed magnet
K. Ohoyama, K. Kurosawa, S. Yoshii, H. Nojiri, Y.H. Matsuda, H. Hiraka, S. Mitsuda(A)IMR, Tohoku Univ., Faculty Science, Tokyo Univ. of Science(A)CNT/ 160μsec/ 146pulse

The reﬂection at the (1/3,1/3,2) position
was observed only in the time region where
the magnetic ﬁeld was larger than 20T.
This is direct evidence that the 3-sublattive
structure is deﬁnitely realised in the phaseof B>20T. In the experiments on AKANE,
we also succeeded in observing the magnetic ﬁeld dependence of 5-sublattice magnetic reﬂection of CuFeO2 under up to 31T;
note that 31T is the highest magnetic ﬁeld
in the world for neutron scattering experiments.
We also tried to observe magnetictransitions in Shastry-Sutherland compound TbB4, which shows metamagnetictransitions for B//[001] in spite of its
Heisenberg-type magnetic structures, on
T1-1. We succeeded in the magnetic ﬁeld
dependence of the 100 magnetic reﬂection which correspond to the antiferromagnetic structure under B=0 T, and conﬁrming the decrescence of the 100 reﬂection
above B=17T.
Since we have conﬁrmed that this magnet
system can generate 40T magnetic ﬁelds
safely, even 40T experiments are feasible bythis system.

15

3-Sub

30

CuFeO2(1/3,1/3,2)
T=4.9K

10

5

20

10

0

Magnetic Field (T)Neutron scattering experiments undermagnetic ﬁeld is indispensable for novel
material science; however, feasible highest
magnetic ﬁelds with conventional superconducting magnets for neutron diffraction
are limited below 13T in Japan, and about
17T in the world, which is not sufﬁcient
to satisfy scientists’ interests. The world
record of magnetic ﬁeld for neutron scattering experiments is B=25T, which was
performed by Motokawa et al. using a
repeating pulsed magnet in Neutron Science Laboratory of High Energy Accelerator Research Organization in Japan. However, neutron scattering experiments over
B=10T are still difﬁcult and limited for thepresent; therefore, easier and more diffusive techniques are ambitioned. Thus, aiming at neutron scattering experiments under B=40T, we are developing easier anddiffusive experimental techniques with acompact pulsed magnet system.
In 2007, we developed a movable magnet
system which consists of a compact condenser bank(C=5.4mF, 3kV) and a mini-coil(diameter:12mm, length:16mm). The coilis installed in a cooling system by liquid
nitrogen, which ican be inserted in an Orange cryostat to cool the sample. The interval of each pulse was reduced to 6-7min.
Neutron diffraction experiments were performed on Kinken spectrometer, AKANE,
and T1-1.
The ﬁrst target material was the triangular lattice compound CuFeO2, whichshows characteristic multi-step matamagnetic transitions for B//c-axis. By using
the developed magnet system, we succeeded in observing induced magnetic reﬂections under pulsed magnetic ﬁelds up
to 31 T on AKANE. Fig.1 shows the timedependence of magnetic ﬁled (solid line)
and intensity of magnetic reﬂection at the(1/3,1/3,2) reciprocal point (open circles).

0
0

1

2

3

4

5

Time (msec)

Fig. 1. Time-dependence of magnetic ﬁeld (solidline) and the intensity of a 3-sublattice magnetic reﬂection observed at (1/3,1/3,2) at T=4.9K on Kinken
neutron spectrometer AKANE (T1-2).

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1-2-18Magnetic structure of an antiferro-octupolar ordering compound
Tb0.94Gd0.06B2C2
E. Matsuoka, Y. Sasaki, D. Usui. K. Ohoyama(A), and H. Onodera
Department of Physics, Tohoku University, (A)Institute for Materials Research, Tohoku
University
The compound TbB2C2 shows an antiferromagnetic (AFM) ordering at TN = 21.7
K with a main [1 0 1/2] propagation vector
and ﬁeld-induced antiferroquadrupolartransitions [1]. The AFM phase in TbB2C2
that has been called phase IV shows someanomalous features in its magnetic behavior. The [1 0 1/2] wave vector in phase
IV is peculiar to TbB2C2 since the other
RB2C2 exhibit [1 0 0]-type AFM structure.
Furthermore, the magnetic susceptibility
anomalously increases below TN without
any spontaneous magnetization. To obtain
more precise information with respect tothe anomalous magnetic behavior, effectsof substitution of Tb3+ ions by Gd3+ havebeen examined and the T-x phase diagramof Tb1-xGdxB2C2 has been constructed [2].
The Gd substitution with a small content(x<0.07) induces drastic change of magnetic properties, namely, an intermediatemagnetic phase named AFM1 appears at
TO<T<TN. Here, TO is a transition temperature from AFM1 to phase IV. In ref.
[2], the following assumption has been proposed: although the magnetic structure of
AFM1 is a [1+delta delta 0]-type long periodic one, the antiferro-octupolar (AFO)
ordering at TO forces to align the magnetic moments with their wave vector of [10 1/2]. The proposed assumption explains
satisfactorily for the anomalous properties
of TbB2C2 and the Gd-substitution effects[2].
To examine the assumption proposed inref. [2], neutron powder diffraction experiments of Tb0.94Gd0.06B2C2 has been performed by using HERMES installed at the
JRR-3M reactor in JAEA. Neutrons with awavelength of 1.82646 A were obtained by
the 331 reﬂection of the Ge monochromator. Since the natural boron is a strong neu-tron absorber, the 11B-enriched boron wasused for the sample preparation.
Fig. 1 shows the neutron diffraction
patterns of Tb0.94Gd0.06B2C2 measured atseveral temperatures. At paramagnetic region (T>TN), all of the Bragg peaks can beindexed as a LaB2C2-type tetragonal structure as shown in Fig. 1(a). On the other
hand, weak satellite peaks around (100)and (101) are observed at 18 K (TO<T<TN)as shown in Fig. 1(b). The positions of thesesatellite peaks are almost identical to thoseobserved in phase IV of TbB2C2 [1] as expected in ref. [2], implying that the magnetic structure of AFM1 is a long periodic
one whose wave vector is [1+delta delta 0]
with delta˜0.11. It is noteworthy that similar long periodic structure is observed forthe intermediate magnetic phase of ErB2C2[3]. In addition to the satellite peaks, strong
magnetic peaks indexed by the wave vectorof [1 0 1/2] are observed at 2.5 K (T<TO)
as shown in Fig. 1(c). The results of present
neutron diffraction support the assumption
proposed in ref. [2].
[1] K. Kaneko et al., J. Phys. Soc. Jpn. 70(2001) 3112.
[2] E. Matsuoka et al., J. Phys. Soc. Jpn. 75(2006) 123707.
[3] K. Ohoyama et al., J. Phys. Soc. Jpn. 71(2002) 1746.

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Fig. 1. Neutron powder diffraction patterns of
Tb0.94Gd0.06B2C2 measured at several temperatures.

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JAEA-Review 2011-050

1-2-19Magnetic structure of multipolar ordering compounds RPd3S4 (R = Ce, Pr)
E. Matsuoka, D. Usui, Y. Sasaki, K. Ohoyama(A), and H. Onodera
Department of Physics, Tohoku University, (A)Institute for Materials Research, Tohoku
University
The rare-earth (R) palladium bronzes
RPd3S4 crystallizes into a cubic NaPt3O4type crystal structure. The R atoms form abody-centered cube and are subjected to a
cubic crystalline electric ﬁeld (CEF) represented by the cubic point group of Th [1].
Systematic studies along the R series haverevealed that the CEF ground states of 4f
electrons in RPd3S4 retain orbital degeneracy [1].
In this system, CePd3S4 shows anomalous magnetic properties: i) despite most
RPd3S4 compounds show an antiferromagnetic (AFM) ordering, CePd3S4 showsa ferromagnetic (FM) one ii) the Curie temperature TC (6.0 K) is larger than the Neeltemperature of R = Gd (5.5 K) [1]. On
the other hand, it has been reported that
PrPd3S4 does not show a magnetic ordering but a multipolar one at TM = 1.56 K [2].
To examine the origin of abovementioned
anomalous properties of CePd3S4 and to
conﬁrm the occurrence of multipolar ordering of PrPd3S4, neutron powder diffraction experiments of CePd3S4 and PrPd3S4
have been performed by using HERMES
installed at the JRR-3M reactor in JAEA.
Neutrons with a wavelength of 1.82646 A
were obtained by the 331 reﬂection of the
Ge monochromator.
The upper panel of Fig. 1 shows theneutron diffraction patterns of CePd3S4. At
9 K (> TC), most peaks can be indexed
as a NaPt3O4-type structure, although thesmall peaks by impurity phase (PdS) arediscernible. At 2.2 K (< TC), two kindsof magnetic Bragg peaks are observed.
One is an AFM component as observed at
15.4 degree indexed as ”AFM100” in theﬁgure. The appearance of (100) magnetic
peak means that the magnetic structure of
CePd3S4 is basically expressed by the wave
vector of [100], i.e., type-I AFM structure as

observed for TbPd3S4 [3]. The other is a FM
component indexed as ”FMhkl”. Therefore,
we can consider that the magnetic structureof CePd3S4 is not a simple FM structure but
a canted-AFM one expressed by two wave
vectors of [100] and [000], which probably
implies that the ordered phase is a coexistent one of AFM and antiferroquadrupolarorder similar to the phase in DyPd3S4 [4].
The lower panel of Fig. 1 shows thediffraction patterns of PrPd3S4 measured
at 3 K (> TM) and 0.7 K (<TM). Unexpectedly, the magnetic Bragg peaks shown as”Mhkl” in the ﬁgure are observed at 0.7
K. All of magnetic peaks can be indexed
by considering a wave vector of [100], thatis, type-I AFM structure is realized below
TM. Note that TM deﬁned by the speciﬁcheat measurements shifts to higher temperatures by magnetic ﬁelds, begins to shift tolower temperatures above 2 T, and disappears above 3.6 T [2]. Such a ”re-entrant”
behavior of TM means that the transition at
TM is not due to magnetic ordering but amultipolar one [2]. To explain the inconsistency between the speciﬁc-heat measurements and the present neutron diffraction,
we now consider that a multipolar ordering (e.g. antiferro-octupolar ordering) occurs at TM and the AFM ordering is concomitant with it.
[1] K. Abe et al., Phys. Rev. Lett. 83 (1999)
5366.
[2] E. Matsuoka et al., J. Phys. Soc. Jpn. 76(2007) 073707.
[3] E. Matsuoka et al., J. Magn. Magn.
Mater. 231 (2001) L23.
[4] L. Keller et al., Phys. Rev. B 70 (2004)
060407.

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Fig. 1. Neutron powder diffraction patterns of
CePd3S4 (upper panel) and PrPd3S4 (lower panel).

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1-2-20Study on low-temperature phase transitions in the Ho3 Al5 O12
R. Morinaga, T. J. Sato, and H. Kimura A
ISSP-NSL Univ. Tokyo, A IMEL NIMS
Geometrically frustrated systems haveattracted special interests for more than
three decades. The antiferromagnetic rareearth(RE) garnet A3 B5 O12 is one of a classical and prototypical frustrated system consisting of three-dimensinally connected triangular motif. The ground-state degeneracy becomes highest for the isotropic magnetic moments such as RE = Gd. Therefore,
Gd3 Ga5 O12 is the most intensively studied for many years. Nevertheless, otherRE garnets have been studied mainly as
the optical matirials; the magnetic study
focusing the effect of geometrical frustration is rather less conducted.From the lowtemperature speciﬁc heat and magnetic
susceptibility measurements of one of RE
garnet Ho3 Al5 O12 , it is known that there
is an antiferromagnetic transition at TN =0.839 K in addition to Weiss temperatureθ Weiss = - 2.92 K [1]. This difference between TN and θ Weiss suggests formation of
the short range antiferromagnetic correlations at TN < T < |θ Weiss |. Last year we
performed neutron powder diffraction andfound the development of magnetic shortrange correlations both in the elastic and inelastic channels.
Here, we report neutron scattering study
on the single crystal Ho3 Al5 O12 . Experiments have been performed at the tripleaxis spectrometer 4G-GPTAS for elastic andC11-HER for low energy inelastic scattering. Single crystals of Ho3 Al5 O12 weregrown by the ﬂoating zone method. Datashown here were taken with a double-axis
mode with incident energy Ei = 14.8 meV at
4G. A single crystal was mounted in a LqHe3 cryostat and cooled down to 0.51 K.
Figure 1 shows the elastic contour mapof two temperature differences between T= 1.3 and 0.51 K in the (H0L) zone. In thisﬁgure, solid lines indicates the Brillouinzone boundary. Strong diffuse scattering is

distributed from magnetic Bragg points tozone center. Furthermore, another type ofdiffuse scattering can be seen around nuclear Bragg peak point 202. However, at
402 nuclear Bragg peak there is no diffuse
scattering. As the diffuse scattering follows
the magnetic form factor and is temperature dependence, magnetic diffuse scattering around 202 originates from the ferromagnetic coupling of the Ho3+ ions. From
the analysis of the powder neutron scattering measurements, the second nearest
neighbor Ho3+ magnetic moments in thesame sublattices have the major contributions to the magnetic diffuse scattering. Detailed analysis is now in progress.
[1] S. Nagata et al. J. Phys. Chem. Solids.
62 (2001) 1123.

Fig. 1. Magnetic diffuse scattering intensity map
S(Q)|T =1.4K - S(Q)|T =0.5K in the (H0L) plane.

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1-2-21

Magnetic and Crystallographic Study on R2CrS4 (R=Ho and Er)
Keitaro Tezuka, Yuta Yoshioka, Seiji Sato, Satoshi Suzuki, Keita Oshikane, Yue Jin Shan,
Hideo, Imoto, and Kenji Ohoyama *Department of Applied Chemistry, Faculty of Engineering, Utsunomiya University,
Utsunomiya 321-8585; *Institute for Materials Research, Tohoku University, Sendai 980-8577
A series of sulﬁdes R2CrS4 (R = Ho-Tm,Y) with the Er2CrS4-type structure (Pca21,
No. 29) gives good examples of the magnetic interactions between Jahn-Teller Cr2+
ions and rare earth ions. Recently we foundthat Y2CrS4 with no magnetic rare-earth
ions showed an antiferromagnetic transition at ca. 65 K while other members of
the series showed magnetic anomalies at
ca. 60 K and also at lower temperatures.
We could reﬁne the magnetic structure of
YCr2S4 at 10 K and of Tm2CrS4 at 3 K.
Both of their magnetic structures have thesame unit cell as their crystal structures
though their magnetic structures are different [1?3].
In this study, neutron diffraction measurements of Ho2CrS4 (80 K, 40 K, 20 K, 9 K,
5 K, and 3 K) and Er2CrS4 (80 K, 50 K, 40
K, and 3 K) were performed on the highefﬁciency and resolution powder diffractometer, HERMES, of Institute for Materials Research, Tohoku University, installedat the JRR-3M Reactor in JAEA (Tokai).
The wavelength of a neutron incident was
1.8265(1) .
Either Ho2CrS4 or Er2CrS4 did not haveany distinct crystallographic phase transition between 80 K and 3 K and were isomorphous with Er2CrS4. At 80 K, cell parameters of Ho2CrS4 and Er2CrS4 were
determined to be a = 12.4990(16) , b =7.4947(9) , and c = 12.4488(17) , anda = 12.4711(13) , b = 7.4718(7) , andc = 12.4399(12) , respectively, which decreased with decreasing temperature. Below the magnetic transition temperatures,ca. 60 K, both compounds showed several
magnetic peaks and their intensities gradually increased with decreasing temperature(see Fig. 1). The magnetic diffractions suggested that paramagnetic chromium andlanthanide ions were ordered as found in
Tm2CrS4. These magnetic peaks could beindexed on the same crystallographic unit
cell (Fig. 1) as observed in Y2CrS4 andTm2CrS4. However, intensities of the magnetic peaks showed that all of the four
members of the series have different magnetic structures.
References[1] K. Tezuka et al., J. Phys. Chem. Solids,
68 (2007), 2133-2137.
[2] K. Tezuka et al., Activity Report on Neutron Scattering Research: Experimental Reports, Vol. 13, nact06-33342.
[3] K. Tezuka et al., Activity Report on Neutron Scattering Research: Experimental Reports, (2007), 214.

Fig. 1. Neutron diffraction patterns of Er2CrS4.

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1-2-22Magnetic structure study of the multi-step metamagnet CeIr3 Si2
Y. Muro(A), K. Motoya(A), K. Shigeto(B), T. Takabatake(B)(A)Department of Physics, Faculty of Science and Technology, Tokyo University of
Science,(B)ADSM, Hiroshima University
CeIr3 Si2 crystallizes in the orthorhombic
ErRh3 Si2 -type structure (Imma, No. 74),
which is a derivative of the hexagonal
CeCo3 B2 -type. The lattice parameters are
a = 7.1765 Å, b = 9.7274 Å and c =5.5971 Å. The results of electrical resistivity, speciﬁc heat and magnetic susceptibility measurements reveal that CeIr3 Si2 is a
Kondo-lattice compound showing two successive magnetic transitions at T N1 =4.1 K
and T N2 =3.3 K[1]. Below 3.3 K, the isothermal magnetization of polycrystalline sample displays mult-step metamagnetic transitions at 0.6 T, 0.9 T and 1.2 T. Recent studyof a single-crystal CeIr3 Si2 has revealed
that the metamagnetic transitions at 0.6 T
and 1.2 T occurs when the magnetic ﬁeld H
applyed along the b-axis while that at 0.9 T
occurs when H//c-axis[2]. We need to obtain the magnetic structures between eachtransition ﬁeld in order to study the origin
of multi-step metamagnetism of CeIr3 Si2 .
Thus we have been carrying out the elastic
neutron scattering of powder and singlecrystal samples.
In order to search magnetic reﬂections,elastic scans were performed in three scattering planes of (HK0), (H0L) and (0KL).
At 1.5 K, we observed four magnetic Bragg
peaks at Q =(0 4/3 ±2/3) and Q =(05/3 ±1/3). Temperature dependence of thepeak at Q =(0 4/3 −2/3) was shown in
Fig. 1(a). The observed magnetic reﬂections agree with those observed in the previous measurement using a powder sample. These non-integer Q’s indicate that thelattice parameters of b- and c-axis below
TN2 becomes three time as large as thoseabove TN1 .
Figure 1(b) shows the temperature dependence of integrated intensity at Q=(04/3 −2/3) and Q=(0 5/3 −1/3). The intensities of all magnetic reﬂections display

a maximum at 2.7 K in spite of no further
phase transition down to 0.5 K. This behavior may indicate the cluster glass-like transition at TN2 possibly due to partial disorder between Ir and Si rigands.
References[1] Y. Muro, Y. Ohno, T. Okada, K. Motoya, J.
Magn. Magn. Mater. 310 (2006), p. 389.
[2] K. Shigetoh, A. Ishida, Y. Ayabe, T. Onimaru, K. Umeo, Y. Muro, K. Motoya, M.
Sera, T. Takabatake, Phys. Rev. B 76 (2007),
p. 184429.

Fig. 1. (a)Temperature dependence of magnetic reﬂection at (0 4/3 -2/3). (b)Temperature dependences of integrated intensity at (0 4/3 -2/3) and (05/3 -1/3).

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1-2-23Magnetic phase diagram of the square lattice CuSb2-xTaxO6 with competinginteractions J1 and J2
M. Nishi, M. Kato(A), K. Hirota(A) and K. Ohyama(B)ISSP Univ. Tokyo, (A) Inorganic Chemistry Lab. Doshisya Univ. (B)IMR Tohoku Univ.
Low-dimensional magnetism of Heisenberg antiferromagnets (HAF) has been afocus of intensive research since discoverof high Tc copper oxides. CuSb2O6 compound has a tri-rutile type structure inwhich Cu2+ ions form a square lattice similar to La2CuO4 [1]. The magnetic susceptibility of CuSb2O6 indicates a typicalbehavior for S=1/2 one-dimensional HAFabove 20K and shows a antiferromagnetic
long-range order at 8.7 K in which Cu spinsare aligned ferromagnetically along b-axis(namely collinear order) with a propagation vector (1/2, 0, 1/2) [2, 3]. If nearest
neighbor coupling J1 is too stronger thannext nearest coupling J2 along diagonal,
Neel order will be stabilized. Then J2 interaction through Cu-O-O-Cu bond is dominant on the collinear order of CuSb2O6.
The substitution of Ta atom instead of Sb
atom causes the decreasing of transition
temperature of long-range order which disappears above x=1 [4]. TaO6 octahedron occupies inter CuO layers and the inter layer
coupling may be decreased with the substitution of Ta atom; x. When J2 coupling
is HAF, there are the spin frustrations between J1 and J2 couplings even if J1 coupling is ferromagnetic or antiferromagnetic[5].
Neutron diffraction measurements of
CuSb2-xTaxO6 powder samples with
x=0.3, 0.7 and 0.8 were carried out on theneutron powder diffractometer HERMES(T13) installed at the JRR-3M reactor at
JAEA. Magnetic Bragg peaks were observed at (1/2, 0, 1/2), (1/2, 0, 3/2) and(3/2, 0, 3/2). Temperature dependencesof Bragg peak for three kinds of samples
were carried out on the neutron triple axis
spectrometer HQR (T11) installed at the
JRR-3M in JAEA. The transition temperature of antiferromagnetic long-range orderwere determined as 8.0K for x=0.0, 3.5K
for x=0.7 and 3.8K for x=0.8. These data
were plot in the ﬁgure 1 with the data ofmagnetic susceptibilities and heat capacities. In comparison of the experimental
results of x=0.7 and 0.8 samples magnetic
Bragg intensity of x=0.8 becomes extremely
weaker than that of x=0.7 in spite of nearlysame Tn. Then it is expected that above
x=0.8 new magnetic phase will be appear.
References[1] A. M. Nakua et al., J. Solid State Chem.
91 (1991) 105.
[2] M. Kato et al., J. Phys. Soc. Jpn. 71S(2002) 187.
[3] B. J. Gibson et al., J. Mag. Mag. Mater.
272-6 (2004) 927.
[4] M. Kato et al., J. Phys. Chem. Sol. 63(2002) 1129.
[5] N. Shanon et al., Eur. Phys. J. B38 (2004)
599.

Fig. 1. Magnetic phase diagram of CuSb2-xTaxO6
obtained by neutron diffraction, heat capacity andmagnetic susceptibility. The antiferromagnetic transition temperature decreases with increasing of substitution of Ta atom.

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1-2-24Competing interactions in two dimensional square lattice CuSb2-xTaxO6
M. Nishi, M. Kato(A), K. Hirota(A) and M. Matsuura
ISSP Univ. of Tokyo, (A)Inorganic Chemistry Lab. Doshisya Univ.
Low-dimensional magnetism of Heisenberg antiferromagnets (HAF) has been afocus of intensive research since discoverof high Tc copper oxides. CuSb2O6 compound has a tri-rutile type structure inwhich Cu2+ ions form a square lattice similar to La2CuO4 [1]. The magnetic susceptibility of CuSb2O6 indicates a typicalbehavior for S=1/2 one-dimensional HAFabove 20K and shows a antiferromagnetic
long-range order at 8.7 K in which Cu spinsare aligned ferromagnetically along b-axis(namely collinear order) with a propagation vector (1/2, 0, 1/2) [2, 3]. If nearest
neighbor coupling J1 is too stronger thannext nearest coupling J2 along diagonal,
Neel order will be stabilized. Then J2 interaction through Cu-O-O-Cu bond is dominant on the collinear order of CuSb2O6.
The substitution of Ta atom instead of Sb
atom causes the decreasing of transition
temperature of long-range order which disappears above x=1 [4]. TaO6 octahedron occupies inter CuO layers and the inter layer
coupling may be decreased with the substitution of Ta atom; x. In this reason we
can study the J1 and J2 couplings about
CuO layer only at the compound with x=1.
When J2 coupling is HAF, there are the spin
frustrations between J1 and J2 couplings
even if J1 coupling is ferromagnetic or antiferromagnetic [5].
Neutron inelastic scattering measurementsof CuSbTaO6 powder samples were carriedout on the neutron triple-axis spectrometer PONTA (5G) and HQR (T11) installedat the JRR-3M reactor at JAEA. Magnetic
excitation peak was observed at Q=0.5A1 for constant E=1.5 meV scan and thisposition shifts to Q=0.55A-1 for constant
E=3.5meV scan at the temperature 1.5K.
CuSbTaO6 powder sample does not become antiferromagnetic long-range orderuntil 1.5K. With the reason that scattering

intensity at Q=0.4A-1 is regarded to background intensity, the magnetic net intensity deducting from the data of Q=0.5A1 to that of Q=0.4A-1 were obtained from
E=0.5meV to 1.7meV with energy resolution 1meV. We found distinctly the spin gap
with E=0.8meV for CuSbTaO6 sample asshown in ﬁgure 1. If there is short-range order, the diffuse scattering is observed usually. Then spin gap of 0.8meV will be comefrom spin frustration mechanism amongmagnetic interactions.
References[1] A. M. Nakua et al., J. Solid State Chem.
91 (1991) 105.
[2] M. Kato et al., J. Phys. Soc. Jpn. 71S(2002) 187.
[3] B. J. Gibson et al., J. Mag. Mag. Mater.
272-6 (2004) 927.
[4] M. Kato et al., J. Phys. Chem. Sol. 63(2002) 1129.
[5] N. Shanon et al., Eur. Phys. J. B38 (2004)
599.

Fig. 1. The experimental results of CuSbTaO6 powder sample in inelastic neutron-scattering. Magnetic
spin gap was distinctly observed at E=0.8meV.

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1-2-25

Crystal Field Excitation of TmAg2In
Takeshi Matsumura
Department of Physics, Graduate School of Science, Tohoku University

A ternary compound RAg2In (R=rare
earth) crystallizes into cubic Heusler-type
structure. This system has a characteristicthat the magnetic ordering temperaturesare very low. Here, in TmAg2In, the speciﬁc heat and magnetic susceptibility measurements have suggested that the groundstate is gamma5 and it has been clariﬁed that the magnetic order does not occur down to 0.5 K. However, the speciﬁcheat exhibits an anomalous peak around 1
K, which is much lower than the 1st excited state at about 15 K. Then, the possibility of Kondo effect has been suggested for
TmAg2In.
The purpose of the present neutron scattering study is to investigate the possibility of Kondo effect in TmAg2In. Determining the crystalline electric ﬁeld (CEF) level
scheme also is another important purpose.
We have performed inelastic neutron scattering experiments on powder sample using TOPAN(6G) and HER(C11) 3-axis spectrometers. First, using TOPAN, we measured the inelastic spectrum up to an energy transfer of 20 meV, and found the CEF
excitation peaks around 1.5 and 2.7 meV.
The spectrum and its temperature dependence was successfully explained by the
CEF model. However, because of the limited energy resolution, it was not possible
to discuss the possibility of Kondo effect.
Next, using HER spectrometer, we measured the spectrum with much higher resolution.
The ﬁgure shows the energy spectrum at
T=0.75 K, below the anomaly of the speciﬁc heat. We can clearly see two CEF excitation peaks at 1.68 meV and at 2.87 meV.
By investigating the temperature dependence, the CEF level scheme has been determined as G 5,1(0)-G 3(19.5)-G 4(33.4)G 1(35.3)-G 5,2(52.8)-G 2(72.5 K), which isexperessed by the parameters of x=-0.013

and W=0.239 K.
Solid line is a ﬁt to the data assuming three Lorentzians at E=0 (quasi-elastic)
and at two CEF levels. At temperatureshigher than 3 K, the data can be well ﬁtted
by this model. However, below 1.5 K, thedata gradually deviate from the Lorentzian
shape, and at 0.75 K, the spectrum cannot
be simply expressed by three Lorentzians.
It also seems that the CEF excitation peaks
are slightly splitted.
A simple scenario is that the CEF levelis slightly modiﬁed (˜ 1 K) by the possible local distortion that reduces the cubic symmetry. Such a disorder can happen in Heusler structure where the Tm
and In sites can exchange relatively easily. At temperatures higher than this splitting, the peak can be expressed by a single
Lorentzian. But at low temperatures, it is
not the case. The width of the peaks about
0.1 meV is comparable to the Kondo temperature estimated by the speciﬁc heat. It isalso a typical value for localized f-electron
systems. It can also be caused by extrinsic
effect of disorder.

Fig. 1.

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1-2-26

Magnetic Structure Analysis in Cr1-xMoxB2 (x = 0.15)
Y. Kousaka(A), E. Kaya(A), H. Kimura(B), Y. Noda(B) and J. Akimitsu(A)(A)Department of Physics and Mathematics Aoyama-Gakuin University, (B)Institute ofMultidisciplinary Research for Advanced Materials Tohoku University
CrB2, which shows a cycloidal magnetic
structure along <1,1,0>, has a hexagonal
AlB2-type structure with a space groupof P6/mmm. With substituting 15 % Mo
to Cr in CrB2, NMR results indicate thatmagnetic structure changes to Spin Density Wave (SDW) [1]. However, it is quite
difﬁcult to explain the change of magnetic
structure by substituting 15 % Mo to Cr
in CrB2, and no other experiments has notbeen performed for decades.
In order to examine the magnetic structure of Cr1-xMoB2, we performed neutron diffraction experiments at the 4-circle
diffractometer T2-2 (FONDER), JRR-3M reactor in JAEA (Tokai). The single crystal
was grown by ﬂoating zone method using
enriched 11B to avoid large absorption of
10B. The data were taken at 10 K. Firstly, we
determined the magnetic propagation vector to be (0.286, 0.286,0). Then, in order todetermine crystal and magnetic structure,
we observed nuclear and magnetic scattering intensities. We corrected the absorption
and extinction effect in nuclear scattering,using DABEX and RADIEL. The crystal
structure was AlB2 structure, which is thesame with CrB2. Fig.1 (a) shows comparison between observed and calculated nuclear structure factors. Determined temperature factors showed negative value, because small contamination of 10B makes
it difﬁcult to estimate absorption coefﬁcient. Though the nuclear structure factors were severely affected by a extinction
effect, the magnetic scattering intensities
were too weak to be affected by the extinction effect. We compared the observed andcalculated magnetic structure factor in cycloid and SDW model. As shown in Fig.1(b), magnetic structure was basically described by the cycloidal structure with 15.8
% of weighted R factor, compared with

SDW structure with 25.3 %.
In order to determine the magnetic structure in detail, we are now analyzing theexperimental results by the use of different magnetic structure like an elipsoidal cycloid structure.
Reference[1] K. Yoshimura et al.: J. Magn. Magn. Matter. 90 (1990) 709.

Fig. 1. Comparison between observed and calculated structure factors.

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1-2-27Chiral Helimagnetism in CuB2O4
Y. Kousaka(A), E. Kaya(A), M. Matsuura(B), K. Hirota(B), M. Nishi(B) and J.
Akimitsu(A)(A)Department of Physics and Mathematics Aoyama-Gakuin University, (B)Institute for Solid
State Physics of the University of Tokyo
Helical magnet copper metaborate
CuB2O4 with the space group I-42d has
been paid attention from the viewpointof chiral helimagnetic ordering. It shows
various magnetic phase transitions at low
temperature: paramagnetic state above TN(= 20 K), commensurate phase with weakferromagnetic ordering in the range of T*(˜ 10 K) < T < TN and incommensurate phase with helimagnetic ordering below T*. In the temperature close to theincommensurate-to-commensurate transition, neutron diffraction experiments show
higher order satellite, which is an evidence
for the formation of magnetic soliton lattice [1]. With increasing an applied magnetic ﬁeld perpendicular to the helical caxis, incommensurate phase II is observedin the region which was supposed to becommensurate magnetic structure [2]. The
magnetic property of CuB2O4 can be interpreted by the lattice chiral XY model:
commensurate-to-incommensurate transition is understood by the formation of chiral magnetic soliton lattice [3]. Moreover,symmetry operation based on its spacegroup, I-42d, allows antiferro-chiral helimagnetic ordering, which alternates rightand left handed screws.
In order to detect the antiferro-chiral helimagnetic ordering, we performed polarization analysis experiments in the incommensurate phase. The single crystal wasgrown by the spontaneous crystallization
technique; slow cooling of CuO, Li2CO3
and B2O3 [3], using enriched 11B2O3 to
avoid the large neutron absorption due to10B. The polarized neutron diffraction experiments were performed at PONTA (5G),
JRR-3M reactor in JAEA (Tokai). The data
was taken at 8 K under an applied magnetic ﬁeld parallel or perpendicular to thescattering vector, due to aligning the neutron polarization parallel or perpendicular to the scattering vector. Accoring to thecalculation of the antiferro-chiral helimagnetic ordered magnetic structure factors in(h, 0, 2h+-q) (h: even), spin ﬂip process
should be observed when the neutron polarization is parallel to the scattering vector. In case of the neutron polarization perpendicular to the scattering vector, nonspin ﬂip process should be observed. However, the experimental results in (2, 0, 4+q) indicates that the both processes are observed in case of parallel and perpendicular neutron polarization. The experimental
data was considered to be affected by several magnetic domains. As this compoundshows commensurate-to-incommensurate
magnetic ordering with cooling temperature, makeing a single magnetic domain incommensurate phase is enough to guarantee the single mangetic domain in incommensurate phase.
Therefore, in order to make a uniform
magnetic domain, we should cool the sample with appling ﬁeld parallel to the b-axis.
Reference[1] B. Roessli et al.: Phys. Rev. Lett. 86 (2001)
1885.
[2] Y. Kousaka et al.: J. Phys. Chem. Sol. 68(2007) 2170.
[3] Y. Kousaka et al.: J. Phys. Soc. Jpn.76(2007) 123709.

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1-2-28Energy Range of Magnetic Excitations in Percolating Two-Dimensional
Heisenberg Antiferromagnet, Rb2Mn0.598Mg0.402F4
S. Itoh and T. J. Sato*High Energy Accelerator Research Organization, Tsukuba 305-0801; *The University of Tokyo,
Tokai 319-1106
Magnetic excitations in the percolating two-dimensional Heisenberg antiferromagnet, Rb2MncMg1-cF4, with c= 0.598
were investigated on the triple-axis spectrometer, GPTAS (4G) at JRR3M in JAEA
(Tokai), in the energy range up to 20 meV.
The magnetic concentration of this system
is very close to the percolation thresholdfor a square lattice (cp = 0.593). The N eltemperature of this system was determined
to be 4 K by measuring the temperaturedependence of the intensity of the magnetic (100) reﬂection. The inelastic spectraat (1+q,0,0) with q = 0 - 0.5 were measured
with a ﬁxed ﬁnal energy Ef = 14.7 meV, at
1.5 K well below TN and at 200 K. The energy resolution was 0.7 meV (FWHM) at
the elastic point.
In 2004 and 2005, we performed similar
experiments to determine the energy rangeof magnetic fractons in this system, andit was reported the observation of dispersive excitations more than 10 meV on GPTAS [1]. However, the peak positions of
the dispersive component were not consistent with the experiments on HER (C1-1) at
JRR3M and on IRIS at ISIS. At present, we
improved the shielding of the spectrometer, GPTAS, and preformed the experiment
again. Figure 1 shows the observed excitation spectrum at the magnetic zone boundary (1.5,0,0) at 1.5 K. The dispersive component at around 12 meV observed in the previous experiment disappeared by the improvement of the shielding, and therefore,
it was found to be spurious. We can still see
a small peak at around 12 meV, and it was
found to be phonon from its temperaturedependence. Therefore, we found the energy range of the magnetic excitations to beless than 10 meV at the present experiment.
Also we previously reported dispersive

excitations observed on HER and on IRIS.
From the result of the precise analysis of thedata taken on IRIS, the observed spectra on
IRIS was found to quantitatively agree withthe predicted dynamical structure factor ofmagnetic fractons [2], and the zone boundary energy of fractons was estimated to beless than 10 meV. And the dispersive spectra observed on HER can be interpreted as
the Ising cluster excitations with a small
dispersion. In the present experiment, we
determined the energy range of the magnetic excitations in this system, and consistently demonstrated the magnetic fractons
and other magnetic excitations.
References[1] S. Itoh et al, Activity Report on Neutron Scattering Research Vol. 13 (ISSP, Univ.
Tokyo 2006).
[2] K. Yakubo et al., J. Phys. Soc. Jpn. 62 (93)2196.

Fig. 1. Excitation spectra at (1+q,0,0) with q=0.5 at
1.5 K in Rb2Mn0.598Mg0.402F4 observed on GPTAS.

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1-2-29Antiferromagnetic ordering of Ca3Ru2O7
Y. Yoshida(A), K. Iwata(B), N. Aso(C), S. Katano(B)(A)AIST, (B)Saitama univ., (C)ISSP-NSL Univ. Tokyo,
Double layered Ruddlesden-Popper (R-P)
type Calcium ruthenate, Ca3Ru2O7, showsan antiferromagnetic ordering below 56K
and a metal-nonmetal transition at 48K.[1]Recent study revealed that Ca3Ru2O7
shows anisotropic behavior in the transport
properties, and is a quasi-two-dimensional
metal below 30K.[2] Powder neutron
diffraction study and thermal expansion
measurement clariﬁed that the transition at
48K accompanies jumps of all lattice parameters.[3,4] As to the magnetic structure of Ca3Ru2O7, it was speculated by themagnetic peak from the powder neutron
diffraction study. In the magnetic groundstate, magnetic moments align ferromagnetically along b-axis within the double
layer and antiferromagnetically between
the double layers.[4] Since the magnetic
anisotropy in the magnetic susceptibility
was changed at the structural transition,
the magnetic structure between 48 and 56K
has not been clariﬁed yet.
In order to clarify the magnetic structureof Ca3Ru2O7, we performed a neutron
diffraction study with a single crystalline
Ca3Ru2O7. Elastic neutron scattering experiments were performed on the tripleaxis spectrometer T1-1 installed at the reactor hall at JRR-3. The incident neutron
wave number was 2.555 -1. The spectrometer was operated with a 2-axis modewith the holizontal collimaitons of G-80’60’. A PG ﬁlter was used to reduce thehigher-order contaminations. The sample
was placed in an aluminum can ﬁlled with
He gas, and mounted in a conventional cryocooler. The nuclear and magnetic peaks
were obtained below 70K.
Besides nuclear peaks, inequivalent 22
magnetic peaks were observed at 10K in
both (0, k, l) and (h, 0, l) planes. Figure 1 shows temperature dependence ofthe peak intensities of the magnetic Bragg(0,0,1) and (0,2,1). With increasing temperature, the peak intensity of (0,0,1) suddenly
decreased at 48K, while that of (0,2,1) increased abruptly. This indicates that the direction of magnetic moments changes fromthe b-axis to the a-axis at the structuraltransition.
[1] G. Cao et al., PRL 78, 1751, (1997).
[2] Y. Yoshida et al., PRB 69, 220411 (2004).
[3] E. Ohmichi et al., PRB 70, 104414 (2004).
[4] Y. Yoshida et al., PRB 72, 054412 (2005).

Fig. 1. Temperature dependence of the peak intensities of (0,0,1) and (0,2,1)

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1-2-30Relationship between Magnetic Structure and Ferroelectricity of LiVCuO4
Y. Yasui, Y. Naito, K. Sato, T. Moyoshi, M. Sato and K. Kakurai*
Dept of Phys., Nagoya Univ., *JAEA
LiVCuO4 has one-dimensional (1D) chainsof the edge-sharing CuO4 squares alongb, which are separated by the nonmagnetic Li+ and V5+ ions. For this system,
the antiferromagnetic transition was foundat TN = 2.4 K, where the dielectric susceptibility epsilon measured along a also
exhibits an anomaly, indicating that theferroelectric transition takes place almost
simultaneously with the magnetic transition. This simultaneous occurrence of thetwo transitions or their coexistence is called
the multiferroic phenomenon [1]. While almost all multiferroic systems ever reported
have the magnetic moments with spin S>1
and/or have more than two magnetic sites,
LiVCuO4 has spins S=1/2 of Cu2+ in the
3d x2-y2 orbital and only one crystallographically distinct Cu site. It is considered
to be the ﬁrst example of spin 1/2 multiferroic systems, which does not bring about
any complications due to the multi-orbital
and multi-site effects in the study of themechanism of the multiferroic nature.
Neutron scattering studies as well as measurements of the dielectric susceptibility
epsilon and ferroelectric polarization P
have been carried out in various magnetic ﬁelds H for single-crystal samples of
LiVCuO4, and the relationship between themagnetic structure and ferroelectricity has
been studied [2]. Neutron scattering measurements were carried out using the triple
axis spectrometer HQR(T1-1), where thedouble axis condition was adopted. For H= 0, the neutron scattering intensities were
measured at Q = (h, k, 0) and (0, k, l) in
the reciprocal space at 1.6 K (<TN) and 5 K(>TN). At 1.6 K, we observed magnetic superlattice reﬂections at Q = (h, k+-delta, 0)and (0, k+-delta, l) (h and l = odd, k = even)with delta=0.466. The magnetic structurethat can reproduce the observed magnetic
scattering intensities, is the ab-plane heli-cal one shown schematically in the ﬁgure.
It is consistent with the structure reported
by Gibson et al.[3]. Considering the ferroelectric polarization P observed along a, wehave found that the relation P=Q*e3 holds,
which is consistent with the existing theories. The ferroelectric polarization along a,
Pa at H=0 is found to be proportional to theneutron magnetic scattering intensity, indicating that the magnetic order is closely related to the appearance of the ferroelectricity.
The behaviors of epsilon and Pa drasticallychange with the applied magnetic ﬁeld.
Neutron diffraction measurements werecarried out in the (0kl) scattering plane under the applied ﬁeld H (//a) and the magnetic structure has been determined, where
the spins have the bc-plane helical structure at least in the region H > 2 T. These results are consistent with the observed suppression of Pa by the applied ﬁeld H along
a above 2 T.
According to the existing theories, the ferroelectricity is expected to be along c forthe bc-plane helical structure. However, wehave not observed the ferroelectricity alongc under the ﬁeld H>2 T applied along a,
where the bc-plane helical structure is actually realized. (Note that Schrettle et al.[4]have reported in the recent paper that theyobserved the weak ferroelectric polarization along c for the bc-plane helical structure.) To understand the origin of this discrepancy remains as a future problem.
References[1] Y. Naito, K. Sato, Y. Yasui, Y. Kobayashi,
Y. Kobayashi, and M. Sato: J. Phys. Soc. Jpn.
76 (2007) 023708.
[2] Y. Yasui, Y. Naito, K. Sato, T. Moyoshi,
M. Sato, and K. Kakurai: to be published in
J. Phys. Soc. Jpn. 77 (2007) No2.
[3] B. J. Gibson et al.: Physica B 350 (2004)

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e253.
[4] F. Schrettle et al.: cond-mat/ 0712.3583.

Fig. 1. The magnetic structure and ferroelectric polarization P of LiVCuO4 (Q and e3 are modulation
vector and helical axis, respectively)

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1-2-31

Magnetic Excitation Spectra of Honeycomb System Na3T2SbO6 (T=Cu, Ni, Co)
Y. Miura, Y. Yasui, T. Moyoshi, M. Sato and K. Kakurai*
Nagoya University, JAEA*
Na3Cu2SbO6 is composed of Cu2SbO6 layers with Na layers between them. The former layers consist of edge-sharing CuO6
octahedra, which form the distorted honeycomb lattice with SbO6 octahedron at thecenter of each hexagon of the CuO6 octahedra (left ﬁgure). The Cu valence is +2 andthe spin S=1/2. The temperature (T) dependences of the spin component of the magnetic susceptibility chi-spin and the speciﬁcheat C-spin indicate that a spin gap exists
in the system. The superexchange interactions between two Cu spins, J1 and J1’ via
Cu-O-Cu paths and that of the Cu-O-O-Cu
path J2 are deﬁned as shown in the left ﬁgure. Taking into account of both the large
Jahn-Teller distortion and the characteristics of the shape of the electron orbits inwhich the spins exist, we expect that J2 isthe largest and J1’ is much smaller thanthe other two, rationalizing that a model ofthe alternating chains along b is a proper
one to describe the present spin system. We
carried out detailed analyses of the spingap behavior using the (chi-spin)-T and(C-spin)-T data, and found, as describedin ref. 1, that the antiferromagnetic (AF)ferromagnetic (F) alternating chain model
successfully describes it.
Inelastic neutron scattering experiments
have been performed on aligned single
crystals of Na3Cu2SbO6 to directly observe the spin-gap in the magnetic excitation spectra. The measurements were carried out on the triplet-axis-spectrometer
ISSP-PONTA at JRR-3 in Tokai. Pyrolytic
graphites (PG) were used as the monochromator and the analyzer. A PG ﬁlter after
the sample was used to suppress the higher
order contaminations. Horizontal collimations were effectively 40’-40’-80’-80’. The
aligned crystals were oriented with the[100] and [010] axes in the scattering plane.
The condition of the ﬁxed ﬁnal neutron en-ergy Ef=14.7 meV was adopted.
Scattering intensities were collected at 10
K by the k-scans along (h, k, 0) with thetransfer energy (E) of 9 meV. Peaks of thesinglet-triplet excitaions were found at thek points of 0.5, 2.5 and 3.5 in the region ofk<4.0 (see the right ﬁgure shown below forh=1). We also carried out similar scans atseveral different values of h and found thatthese peaks extend along h, having the onedimensional character of the spin system,
which is consistent with the above description that the system can be understood by
the AF-F alternating chain model. Then, theE-scan proﬁles were obtained at Q=(1, 2.5,0) at several ﬁxed temperatures in the region of 10<T<200 K, where the gap energy
were found to be 9 meV, which also agreed
with the results obtained by our previous
studies of chi-spin and C-spin.
The dispersion curve was also measured by
the E-scans at various Q points. Analyses toestimate the J1 and J2 values from the dispersion curves are underway.
[1]Y. Miura et al.: J. Phys. Soc. Jpn. 75 (2006)
084707.

Fig. 1. (Left) Schematic ﬁgure of the honeycomb
layer. At the corners of the octahedra, O atoms exist, and a Cu or Sb atom is within each octahedron.
(Right) The Q-scan proﬁle of (1, k, 0) at 10 K for E=9
meV.

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Neutron diﬀraction studies on a Pr7Ni3 single crystal
T. Tsutaoka(A), A. Tanaka(A), Y. Andoh(B), A. Tada(C), G. Nakamoto(C) and
M. Kurisu(C)(A)Graduate School of Education, Hiroshima University, Hiroshima 739-8524, Japan(B)Faculty of Regional Sciences, Tottori University, Tottori 680-8551, Japan(C)Japan Advanced Institute of Science and Technology, Ishikawa 923-1292, JapanThe rare earth compound Pr7Ni3 crystallizes in the hexagonal Th7Fe3 type structure with the space group P63mc [1]. Fromthe magnetic measurements, it possesses
the two magnetically ordered states; oneis an antiferromagnetic state between TN= 4.2 K and Tt = 2.1 K and ferrimagnetic
like state below Tt. [2]. In this study, neutron diffraction measurements have been
carried out on a Pr7Ni3 single crystal in thea* - c* reciprocal plane using the HQR spectrometer of JRR-3M of in the temperature
range from 1.5 to 10 K.
Figure 1(a) shows the magnetic and nuclear reﬂections in the a* - c* reciprocal
plane at 1.5 K. The magnetic reﬂections appear at the positions indexed by the propagation vector k = (0.5, 0, 0). A magnetic
reﬂection was also observed at the nuclear
position (1, 0, 0) indicating a small spontaneous magnetization along the c-axis. Ferrimagnetic magnetization curve is also observed at 1.9 K [2]; a canted magnetic structure along the c-axis can be possible.
Figure 1(b) shows the intensity of the magnetic reﬂection at (0.5, 0, 2) and (1, 0, 0) as afunction of temperature. The magnetic reﬂection at (0.5, 0, 2) shows a maximum at
Tt and decreases; it disappears around TN.
On the other hand, the ferromagnetic component at (1, 0, 0) disappears at Tt. The kx
was constant up to TN.
Magnetic structure analysis using a Rietveld method for each state is now inprogress.
References[1] G. L. Olcese, J. Less-Common Met. 33(1973) 71.
[2] Y. Haga et al., Meeting Abstracts of the
Phys. Soc. Jpn. 62, 1-3 (2007) 420.

Fig. 1. Magnetic and nuclear reﬂections of a Pr7Ni3
single crystal in the a* - c* reciprocal plane at 1.5
K (a). The intensity of (0.5, 0, 2) magnetic reﬂection
and the magnetic component of (1, 0, 0) as a functionof temperature (b).

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Neutron Diﬀraction Studies on Y7Rh3Dx
T. Tsutaoka(A), A. Tanaka(A), A. Tada(B), G. Nakamoto(B), M. Kurisu(B) and
Y. Andoh(C)(A)Graduate School of Education, Hiroshima University, Hiroshima 739-8524, Japan(B)Japan Advanced Institute of Science and Technology, Ishikawa 923-1292, Japan(C)Faculty of Regional Sciences, Tottori University, Tottori 680-8551, JapanThe rare earth intermetallic compounds
R7Rh3 based hydrides can have the hexagonal Th7Fe3 type structure with the spacegroup P63mc in the relatively high hydrogen content up to R7Rh3H30[1]. Magnetic property of the Tb7Rh3 and Dy7Rh3changes from antiferromagnetic to ferromagnetic and the electrical propertychanges from semimetallic to metallic by
the hydrogenation[1]. We have carried out
the neutron diffraction experiments forthe parent compounds and their deutrids
R7Rh3Dx (R = Dy and Ho) [2]. In thisstudy, we have performed powder neutron diffraction measurements on the nonmagnetic deutride Y7Rh3D20 to investigate the deuterium conﬁguration. Neutron
diffraction measurements have been carried out by using the HERMES spectrometer of JRR-3M in the temperature range
from 10 to 100 K with a wave length of
1.82645(6) A. The data were collected by an
MFC mode.
Figure 1(a) shows the powder neutron
diffraction proﬁles of Y7Rh3 at 10 K.
All peaks in Y7Rh3 can be indexed by
the Fe7Rh3 type structure and the lattice paramters and atomic positions werereﬁned. Obtained lattice parameters are
a=9.772(5) and c=6.174(4), respectively.
Figure 1(b) shows the powder neutron
diffraction proﬁle of Y7Rh3D20 at 16 K. The
simulation result with the expanded lattice
parameter a=10.246 and c=6.626, which isdetermined from X-ray diffraction analysis, and diffraction peak positions are also
indicated. In the Y7Rh3D20, all peaks for
Th7Fe3 type structure were shifted toward
lower angle side indicating the lattice expansion; the diffraction pattern is different from Y7Rh3. Three diffraction peaks,

which are indicated by the vertical arrows,
can not be indexed by the Th7Fe3 typestructure. Thus these diffraction peaks canbe from the deuterium conﬁguration. The
analysis of the crystal structure and thedeuterium conﬁguration of Y7Rh3Dx with
the Rietveld analysis are now in progress.
References[1] R. Sato, T. Tsutaoka, S.M. Filipek, J. Alloys and Comp., 446-447 (2007) 610.
[2] T. Tsutaoka et al., Activity report on
Neutron Scattering Research, Report #120
(2006).

Fig. 1. Neutron diffraction proﬁles for Y7Rh3(a) and Y7Rh3D20. Simulation result with the expanded lattice parameter a = 10.246, c =6.626 anddiffraction peak positions are also indicated.

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1-2-34Magnetic excitation spectrum in the frustrated triangular lattice antiferromagnet
CuFe1-xAlxO2
S. Mitsuda, T. Nakajima, S. Iwamoto, N. Terada1
Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601, Japan,
1 ICYS, National Institute for Materials Science, Ibaraki 305-0044, Japan
Magnetic oxide CuFe1-xAlxO2 has been
extensively investigated to elucidate thespin-polarization coupling in the ferroelectric incommensurate (FEIC) phase that ismagnetic ﬁeld- or impurity-induced (seeFig.1 b) from the 4-sublattice ground state.
Beyond multiferroic study on static coupling between spin and electric polarization, we have started inelastic neutron scattering study, aiming to investigate its dynamical spin-polarization coupling. However, since higher-temperaturepartially disordered (PD) state is spatially co-existing in the FEIC phase at low
temperature, quantitative inelastic neutron
scattering measurement in the FEIC phase
under zero magnetic ﬁeld has been difﬁcultfor the Al-doped CuFeO2, although PDcontamination-free FEIC phase can be obtained by transverse magnetic ﬁeld cooling[1].
Taking accounts of that coexistence of
PD state might be due to local distortion
around doped Al3+ ions with smaller ionicradius than that of Fe3+, we newly choose
Ga-doped system, CuFe1-xGaxO2, whereionic radius of doped Ga3+ ions seems to
be close to that of Fe3+. As was in previous studies on CuFe1-xAlxO2 [2-3], we
performed elastic as well as inelastic neutron scattering measurements on the single crystal CuFe1-xGaxO2 sample with x= 0.35, using the triple-axis neutron spectrometer HER(C1-1) installed at JRR-3.
As shown in Fig.1 a, diffraction proﬁle of magnetic (q, q, 1.5) reﬂection in
the FEIC phase is resolution-limited single peak as is in the OPD phase, clearlysuggesting that the FEIC phase in Gadoped system, CuFe1-xGaxO2, is PDcontamination-free. Actually, the discontinuous phase transition between PD stateand FEIC state is quite sharp. Adapting
magnetic phase transition temperatures
obtained from present experiment to themagnetic phase diagram of CuFe1-xAlxO2,
Ga-doping with x=0.035 effectively corresponds to Al-doping with x=0.019 as isshown in Fig.1 b. Since, in preliminary
inelastic measurement on the Ga-doped
system, relatively clear magnetic excitation spectrum than that in previous measurement [3] has been observed, further
systematic inelastic study using Ga-doped
system is desired.
References[1] T. Nakajima et al.: JPSJ 76 (2007) 043709,[2] N. Terada et al.:JPSJ 74 (2005) 2604,[3] N. Terada et al.: JPCM 19(2007) 145241.

Fig. 1. (a) magnetic diffraction proﬁles for PD
and FEIC state,(b) x-T magnetic phase diagram of
CuFe1-xAlxO2[2]Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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1-2-35Magnetic Structure of Noncentrosymmetric heavy-Fermion Ce4 Ni3 Pb4
T. Onimaru1 , K. Shigetoh1 , A. Ishida1 , and T. Takabatake1,2
1 AdSM, Hiroshima Univ., 2 IAMR, Hiroshima Univ.
Cerium-based ternary intermetallic compound Ce4 Ni3 Pb4 crystallizes in the trigonal La4 Ni3 Pb4 -type structure (space groupR3) without inversion symmetry.[1] The
lattice parameters are a=9.931 Å andc=9.464 Å. In the unit cell, the Ce atoms
contain 9b and 3a sites, the Ni atoms 9b,
and the Pb atoms 9b and 3a sites, respectively. Magnetic property of polycrystalline
Ce4 Ni3 Pb4 has already been reported by
Shigetoh et al.[2] Both the temperature dependence of the speciﬁc heat and electric
resistivity show anomalies at TM =4 K and
TN =3 K. M/B shows no anomaly at TM ,however, it exhibits a considerable increase
below TN in magnetic ﬁelds of B<1 T.
This ferromagnetic-like behavior probably
results from the Dzyaloshinsky-Moriya interaction due to the lack of the inversion
symmetry. In much higher magnetic ﬁelds
than 1 T, a characteristic peak due to an antiferromagnetic transition appears.
To determine a magnetic structure of
Ce4 Ni3 Pb4 , We have performed neutron
diffraction experiments on a powder sample and a single-crystalline one. The powder neutron diffraction experiments were
performed with the ISSP triple-axis diffractometer HQR(T1-1) . The sample wasmounted at a coldhead of an 1K refrigerator and cooled down to 0.74 K. Fig.
?? shows results of the powder neutron
diffraction experiments at T =0.74 K and
7.0 K . Difference between the diffraction
patterns at T =0.74 K and 7.0 K is appearance of superlattice reﬂection labeled”Mag.” in the ﬁgure at around the scattering angle of 2θ =18.1 deg which should−1
be corresponding to |Q|=0.80 Å
. In
the temperature dependence of the intensity, the intensity decreases with increasing temperatures and reaches to the background intensity at around 3 K corresponding to TN . Above 3 K, no difference be-

tween the patterns at 0.74 K and 7 K was
observed. Furthermore, in order to determine a propagation vector of the magnetic structure, we performed the neutron
diffraction measurements on the singlecrysalline sample using the ISSP triple-axis
spectrometer GPTAS(4G). The sample wasmounted at a coldhead of an Orange cryostat and cooled down to 1.4 K. Searches
for the position of the superlattice reﬂection
were performed on the scattering plane ofthe (H0L), (HHL) and (0KL). Below 3 K,
it appears at Q=(0, 1, 1/2) and its equivalents, suggesting that an antiferromagnetictransition should occur at around TN =3 K.
The determination of the magnetic structure is now in progress.
References[1] L. D. Gulay et al.: J. Alloys Compd. 392(2005) 165.
[2] K. Shigetoh et al.: J. Phys. Soc. Jpn. 75 (2006)
033701.

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Crystal and magnetic structures of 12L-perovskites Ba4LnRu3O12 (Ln = Pr andTb)
Shimoda Y., Doi Y., and Hinatsu Y.
Division of Chemistry, Graduate School of Science, Hokkaido University
Crystal structure and magnetic propertiesof new perovskites Ba4LnRu3O12 (Ln = Pr
and Tb) were investigated. The schematic
crystal structure is illustrated in Fig. 1.
In this structure, two kinds of the B siteions, Ru and M, occupy the face-sharing
octahedral sites (Ru3O12 trimer) and thecorner-sharing octahedral ones (LnO6 octahedron), respectively. From the magnetic
susceptibility and speciﬁc heat measurements, it is found that both compounds
show magnetic anomalies at low temperatures.
In order to determine their crystal andmagnetic structures, the neutron diffraction measurements were performed using
the high efﬁciency and resolution powder diffractometer, HERMES, of Institutefor Materials Research, Tohoku University,
installed at the JRR-3M Reactor in JAEA
(Tokai). The wavelength of a neutron incident is 1.82035 . The data were analyzed
by the Rietveld technique.
As results of the Rietveld analyses of
the neutron diffraction data at room
temperature, the crystal structures of
Ba4LnRu3O12 (Ln = Pr and Tb) were
determined. Both compounds have aperovskite-related structure which consistsof the 12-layer (12L) of the BaO3 sheets.
The Ba4TbRu3O12 has a hexagonal unit
cell with space group R-3/m; the cell paand c = 29.0212
rameters are a = 5.8314. On the other hand, the crystal structureof the Ba4PrRu3O12 is monoclinically(space group C2/m) distorted with a =10.157 , b = 5.869 , c = 29.315 , andbeta = 90.910 degree.
The neutron diffraction measurements at
low temperatures were performed for
Ba4TbRu3O12. In the diffraction proﬁle at
2.5 K, some additional reﬂection peaks
were found at lower angles, which were

not observed at room temperature. Thesepeaks can be indexed using a propagation vector k = (0, 0, 3/2). The magnetic structure was by the Rietveld analysis of the data. In this magnetic structure,
the magnetic moments of Ru ions in the
Ru3O12 trimer order antiferromagnetically(up-down-up). The ferrimagnetic moments
remaining in the Ru3O12 trimers and magnetic moments of Tb ions order antiferromagnetically along the c-axis.

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Magnetic excitations in MCr2 O4 (M=Fe, Ni)
K. Tomiyasu1 , H. Hiraka2 , K. Ohoyama2 , and K. Yamada1
WPI-AIMR Tohoku Univ.1 and IMR Tohoku Univ.2

The geometric frustration is expanded toeven the systems with magnetic moments
on a non-frustrated sub-lattice in addition
to a frustrated one. In the spinel chromites,
MCr2 O4 (M=Mn, Fe, Co, Ni, Cu, Zn, Mg,
Cd, Hg), the M ions and the Cr3+ (S=3/2)
ions occupy the non-frustrated A sites (diamond) and the frustrated B sites (corner sharing tetrahedra), respectively. The
chromites with nonmagnetic ions M=Zn,
Mg, Cd, Hg at A sites are well known as
the highly frustrated systems, but the materials with magnetic and non-Jahn-Teller
ions M=Mn and Co exhibit the simultaneous formation of long-range ferrimagnetic
order and short-range spiral order, meaning the partial frustration.
Meanwhile, the other ions M=Fe, Ni, Cu
lead to only the long-range magnetic order because of the large Jahn-Teller distortion (3-10%), which should eliminate thegeometric frustration. However, ZnCr2 O4
and MgCr2 O4 exhibit the anomalous spin
excitations without dispersion at 4.5 meVaround Q=1.5 Å−1 by powder neutron inelastic scattering even in the tetragonal andantiferromagnetic ordered phase. Therefore, we also suspected that such excitations are hidden in the FeCr2 O4 , NiCr2 O4
and CuCr2 O4 . In the present experiments,
we performed the elastic and inelastic scattering experiments on the powder specimens of FeCr2 O4 and NiCr2 O4 on HERMES and AKANE.
Figures 1(a) and 1(b) show the data ofS( Q) on FeCr2 O4 and NiCr2 O4 at 12 K, respectively. The appreciable signal of magnetic diffuse scattering is observed around
Q=1.5 Å−1 in both of the materials. Figures 1(c) and 1(d) show the data of S( Q, E)
on the two materials, respectively. It isrevealed that the diffuse scattering, measured in the diffraction experiments, comesfrom the component of inelastic scattering

around 6 and 5.5 meV, respectively. The
excitations are almost non-dispersive, andthe energy is roughly comparable to thatof Zn/MgCr2 O4 , suggesting that the magnetic modes in the different systems are
the same in origin. We have clariﬁed themode in MgCr2 O4 to be the antiferromagnetic hexamer, which is the same as in
the paramagnetic phase, in another experiments on a single-crystal specimen in thelast year and is emblematic of the geometric frustration. Thus, it is becoming plausible that even the Jahn-Teller materials also
exhibit the geometric frustration as the inelastic component with a ﬁnite gap energy.

Fig. 1. Present neutron scattering data on powder
speciments of FeCr2 O4 and NiCr2 O4 .

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1-2-38Spin Waves in MnPS. Yano(1), Y. Kousaka(1), M. Nishi(2), M. Matsuura(2), K. Hirota(2) and J. Akimitsu(1)(1)Department of Physics and Mathematics, Aoyama-Gakuin Univ., 5-10-1 Fuchinobe,
Sagamihara, (2) Institute for Solid State Physics, The Univ. of Tokyo 106-1 Shirakata, Tokai
319-1106
Manganese phosphide MnP is a ferromagnetic intermetallic compound below TC =291K, and it transforms into a proper screw
spiral state at T* = 47K.
The crystal structure is a slightly distorted
NiAs structure with the lattice parametersof a = 5.916 Å, b = 5.260 Å, c = 3.173 Åat room temperature. In the ferromagnetic
state, the easy-axis of the magnetization isthe c-axis. In the spiral state, the spin rotates in the b-c plane with a propagation
vector 0.117a* along the a-axis.
The ferromagnetic spin-waves along thethree principal axes had been measured by
Todate et al[1]. They reported that the dispersion relation along the a-axis exhibits
anomalous wave vector and temperaturedependences, and also the quadratic q dependence was observed along both the band c-axis. However, the measurements
were taken only in ferromagnetic state, sothat the information about the spiral stateis still missing.
In order to elucidate the mechanism of the
spiral state, the information of spin wave
in the whole Brillouin zone is crucially important. We focus our attention on the spinwave dispersion of the spiral state in MnP,in order to investigate the magnetic mechanism of the spiral state.
We performed the neutron inelastic scattering experiments at triple-axis spectrometer PONTA (5G), JRR-3M reactor in JAERI(Tokai).
The single crystal of MnP, whose size islength 40mm × diameter 9mm was grownby the Bridgman method.
The measurements were taken at 18 K, as
shown Fig1 and Fig2, the spin wave dispersions have been mearsured along thea- and b-axis. From these experimental results, however, it is difﬁcult for to ob-tain the precise exchange parameters ofmagnetic interaction. Additional measurements are needed to determine the magnetic exchange parameters.
Further measurements of spin waves atlarge-q and ω region are now in progress.
References[1] Y Todate et al.: Jou Phys Soc Jpn. 56 36(1987).

Fig. 1. Spin wave relations along the a- and b-axis

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1-2-39
1-2-39Magnetic structures and transitions of HoRh2Si2
T. Shigeoka(A), H. Shibasaki(A), T. Fujiwara(A), M. Nishi(B)(A) Grad. Sch. of Sci. Eng. Yamaguchi Univ, (B) ISSP Univ. of Tokyo
Neutron diffraction measurements by
Slaski et al. have revealed that the ternarycompound HoRh2Si2, having the tetragonal ThCr2Si2-type crystal structure(space group: I4/mmm), orders antiferromagnetically below TN=27 K [1]. The
antiferromagnetic structure reported ischaracterized by the wave vector k= (0,0, 1), having Ho moments tilted by 28+-3
degree from the c-axis. Recent magnetic
study shows that HoRh2Si2 has threetransitions: T1=12.4 K, T2=27.5 K and
TN=29.5 K. The magnetic structures havebeen, however, unknown yet.
In order to investigate the magnetic
structures for each temperature region:
T<T1 ,T1<T<T2 and T2<T<TN, neutron
diffraction studies have been performed on
a HoRh2Si2 single crystal using the triple
axis spectrometer HQR installed at JAERI,
Tokai, Japan. The a-axis of the single crystal was vertically oriented to obtain the distribution of neutron intensities in the a*-c*
reciprocal plane.
The single crystal has been grown by
the tri-arc Czochralski method. The single
phase nature has been conﬁrmed by X-ray
powder diffraction
At low temperatures below T1, an appearance of antiferromagnetic reﬂections associated with the propagation vector k= (0,0, 1) has been conﬁrmed. Both (001) and(100) reﬂections are observed, indicatingthat magnetic moments tilt from the c- anda-axis. This result is consistent with theprevious report [1]. An analysis for magnetic structure for low temperature is now
in progress. The temperature dependenceof peak intensity for antiferromagnetic reﬂections (001) and (100) is shown in Fig.
1. The (001) reﬂection disappears above
T1. The temperature dependency of intensity of (100) peak changes at T1. In intermediate temperature region T1<T<T2,

only antiferromagnetic reﬂections associated with the AFI-type structure are observed. All magnetic reﬂections disappear
above T2; for T2<T<TN, magnetic reﬂections could not detected at all. We believethat new magnetic reﬂections should appear for T1<T<T2 and T2<T<TN. Further
neutron study should be required.
[1] M. Slaski et al., J. Magn. Magn. Mat.
39(1983)268.

Fig. 1. Temperature dependence of antiferromagnetic (001) and (100) peak intennsity of HoRh2Si2

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Neutron scattering study on the molecular magnet Mn6Sb2
Kazuki Iida and Taku J SatoISSP
the innter-cluster exchange interaction between Mn6 Sb2 cluster with S = 15 asa perturbation to inner-cluster Heisenberg
model. Taking account of the layered triangular structure of the Mn6 Sb2 system, wefound that antiferromagnetic short-rangespin correlations on the triangular lattice
reproduce the observed diffuse scattering
pattern. The Q dependence of the 0.26 meVpeak is also reproduced as the elementary
excitation in the short-range ordered cluster spins. Thus the inter-cluster interaction
can explain not only the diffuse scattering
but also the peak at 0.26 meV.
Ferromagnetic inter-cluster interactions
have been know in the magnetic molecules,
such as in Mn12 where inter-cluster interactions give rise to the long-range magnetic
order. However, the antiferromagnetic interactions were quite rare; Mn6 Sb2 is theﬁrst system in which antiferromagnetic interactions are conﬁrmed by the neutron
spectroscopy. The inter-cluster interactionis the second-dominant term which does
not perturb the inner-cluster ferromagnetic
coupling (i.e., S = 15 is the ground stateeven with the inter-cluster coupling). Since
the cluster spin forms 2D triangular net, theintrinsic geometrical frustration may prohibits the long-range order in the Mn6 Sb2
system.
Intensity (counts/7min.)Mn6 Sb2 is a molecular magnet. Mn2+
ions with s = 5/2 are forming a approximately eqational hexagon and coupled by ferromagnetic exchange interaction between nearest neighbor ions, and theground state is S = 15.
We performed inelastic neutron scattering experiments and succeeded to observe
the magnetic excitations. There were two
inelastic peak at 0.26 and 0.54 meV in
the inelastic neutron scattering spectrum at
1.5 K. They are conﬁrmed to be magnetic
excitations from their temperature dependences and Q dependences. On the other
hand, magnetic susceptility result expects
that the ﬁrst excitation mode from S = 15
to 14 exists at 0.52 meV. We measure the Qscans at the peak energies 0, 0.26 and 0.54
meV, and at two temperatures 1.5 and 6.0
K. Fig. 1 shows the temperature subtractions of the obtained Q-scans. The Q dependence of 0.26 meV is different from thatof 0.54 meV. Thus, the inner-cluster Heisenberg Hamiltonian cannot explain the peak
at 0.26 meV. At the elastic position, diffuse
scattering was observed shown in Fig. 1,
and its shape is good agreement with the Q
dependence of 0.26 meV. This fact suggeststhat a short-range correlation is developed
at low temperature and have the excitation
mode at 0.26 meV.
The peak of diffuse scattering is at Q =0.2 A−1 , corresponding to 2π/0.2 ∼ 30 A
in real space which is comparable with the
distance between Mn6 Sb2 clusters. We suppose that there are antiferromagnetic interaction between cluster spins (S = 15), resulting in the diffuse scattering. The origin of the inter-cluster interactions may
be the dipole and/or exchange interactions. D, the constance of a dipole interaction is ( gμ B )2 /R3 = 0.028 μeV, andthus the dipole interaction cannot accountfor the peak at 0.26 meV. Hence we add

400

2000
G-O-BeF-S-RC3-BeF-20mm
0.26 meV
0.54 meVelastic (right axis)

300

200

1500
1000
500
0

100
-500
0
0

0.2

0.4

0.6

0.8

-1

1.0

1.2

1.4

-1000
1.6

Q (Å )

Fig. 1. The subtractions of Q dependency at 6.0 K
from that at 1.5 K of 0.26, 0.54 and 0 meVActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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Neutron scattering in Ba2 MnGe2 O7
T. Masuda, S. Kitaoka and M. Nishia
International Graduate Schools of Arts and Sciences, Yokohama City University,
22-2 Seto, Kanazawa-ku, Yokohama, 236-0027, a Neutron Scattering Laboratory, Institute for Solid State Physics,
University of Tokyo, 106-1 Shirakata, Tokai, Ibaraki, 319-1106, Japan
Ba2 MnGe2 O7 is an ideal 2D squarelattice antiferromagnet (AFM) with Mn2+
spin of S = 5/2. The crystal structure is
tetragonal with space group P − 421m, a =8.4952 Å, and c = 5.5256 Å. From the magnetic susceptibility measurement the antiferromagnetic (AF) exchange interaction isestimated to be J ∼ 0.05 meV. The spinwave calculation based on the obtained parameter predicts that the boundary energy
would be about 0.8 meV; ideal energy scale
for cold neutron scattering. This magnetic
energy scale is also adequate for high magnetic ﬁeld study. Since the saturation ﬁeld
is estimated to be 10 T, the exotic behaviorof the spin dynamics in very high ﬁeld[2]could be observed by using conventional
superconducting magnet. Hence it is important to study the basic magnetic property of Ba2 MnGe2 O7 in zero ﬁeld as the ﬁrst
step of study in spin dynamics in high magnetic ﬁeld. We performed magnetic diffraction in 5G PONTA and also in T11 HQR.
The crystal is cylindrical shape with φ7mm × 7mm. Since the isostructural compound Ba2 CuGe2 O7 [1] is well known as
spiral magnet with Dzyaloshinskii-Moriya
and KSEA interaction with the propagation vector of (1 − ζ 1 − ζ 0), we searched
the magnetic Bragg peak in the scattering
plane of (hk0) in the ﬁrst experiment 5G.
However any magnetic signal was not detected. Then we try next experiment in(h 0 l ) plane in T11. The experimental
set up was Guide - 40 - PG ﬁlter - sample - 40  - 60 . To our surprise we foundthe magnetic peak at commensurate position of (h 0 n/2) (n is integer.) We collected 10 inequivalent magnetic peaks and
we are now doing magnetic structure analysis. Next we performed inelastic neutron

scattering in C11 HER. The sample size is
φ7 mm × 40 mm. The experimental setp up
was guide - open - Be ﬁlter - sample - 80
- 80  with e f = 3meV. We performed a series of constant q scans in the (h 0 l ) plane.
We observed well deﬁned magnetic excitation in h̄ω ≤ 0.6 meV. The obtained dispersion relation is shown in Fig. ??. The data
is well explained by weakly coupled squarelattice AFM with weak diagonal interaction
with the exchange parameters of J1 = 0.029
meV, J2 = 0.0015 meV, and Jinter = 0.0007
meV. Here J1 is main interaction, J2 is diagonal interaction, and Jinter is interplane interaction. As is deduced from crystal structure and bulk magnetic susceptibility measurement, Ba2 MnGe2 O7 is an ideal squarelattice AFM with moderate energy scale forboth neutron scattering and magnetic ﬁeld
study.
References[1] A. Zheludev et al., Phys. Rev. B 54, 1563
(1997).
[2] Z. E. Zhitomirsky et al., Phys. Rev. Lett. 82,4536 (1999).

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Fig. 1. The magnetic dispersion of Ba2 MnGe2 O7 .
The solid line is the ﬁtting by SW calculation.

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Neutron scattering in O2 adsorbed CPL-1
T. Masuda and K. Hirotaa
International Graduate Schools of Arts and Sciences, Yokohama City University,
22-2 Seto, Kanazawa-ku, Yokohama, 236-0027
a Neutron Scattering Laboratory, Institute for Solid State Physics,
University of Tokyo, 106-1 Shirakata, Tokai, Ibaraki, 319-1106, Japanthe difference is, the absolute intensity ofthe background is large and we have toredo the background measurements. This
is why we obtained only preliminary datain the year of 2006. Figure 1 was the bestdata.
In the year of 2007 we know exactly what
we need and what we should do. We focused on obtaining publication quality datain (i) a series of constant q scans at T = 2
K (4 days), (ii) constant energy scan at 8
meV (4 days), and (iii) a constant q scans
at various temperatures (4 days). We successfully collected the data set. The detailof this study will appear in a forthcoming
publication.
Now we have some technique and budget to obtain deuterated samples. In thenext ﬁscal year we will proceed the project
more efﬁciently.
References[1] R. Kitagawa, et al., Science 20, 2358 (2002).
[2] T. C. Kobayashi et al., Prog. Theor. Phys.
Suppl. 159, 271 (2005).
open-80-CPL(O2)-PG-RadCol.-HFA-open
Ef=14.7meV(Const e scan at hw=8meV) - (Const e scan at hw=6meV)

4000

Intensity (counts/4 min.)

Oxygen is a rare diatomic magnetic
molecule. Recently trial to utilize the oxygen as magnetic entity has been conductedin some types of nanoporous metal-organic
compounds. The physically adsorbed O2
molecule forms magnetic framework andO2 based magnet is realized. Amongthem in CPL-1 (C16 H12 Cu2 N6 O10 ) [1], O2
molecules forms ladder-like structure andthe spin-gap behavior is expected. Indeed
the magnetic susceptibility [1] and magnetization measurements [2] suggests thespin gap of 60 ∼ 88 K (5.2 ∼ 7.6 meV).
Hence we started the thermal neutron
scattering study on the O2 based magnet
since the ﬁscal year of 2006. We succeededin observing the magnetic signal of the adsorbed oxygen and obtained preliminary
data set of constant q scans and constantE scans (Fig.1). The difﬁculty of the study
was that we had to collect all the data set in
one allocated machine time due to the following technical reason.
The sample contains many hydrogenatoms and the background is large. Therefore, we performed scans on non-O2 adsorbed sample for background measurement and then we repeat the same scan on
O2 adsorbed sample. It is not until we ﬁnish a set of scans that we obtain the net
magnetic excitation of the adsorbed oxygen. Usually we noticed that some additional scans were necessary in the end ofexperiment. In the next allocated experiment we found that the obtained background was slightly different from that in
the previous one. This is probably due toslightly different instrumental conﬁguration; e.g., effective volume of the sample inthe specially designed Al can, detailed optical set up, and so on. Even though small

Const E scan
Const Q scan

3000

2000

1000

0

0

1

2

3

4

5

-1

q (A )

Fig. 1. Constant E scan.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 629

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JAEA-Review 2011-050

1-2-43

Powder diﬀraction study on the ternary compound Ce5 Ni2 Si3
T. J. Sato, K. Iida, H. Kitazawa1 , and Y. S. Kwon2
ISSP-NSL, University of Tokyo, Tokai, Ibaraki 319-1106, Japan
1 NIMS, Tukuba, Ibaraki 305-0047, Japan
2 Department of Physics, Sung Kyun Kwan University, Suwon 440-476, Korea

Intensity (counts)

tures 2 K and 15 K. The overall diffraction
patterns are mostly the same for two temperatures, inferring absence of the structural transition. At the lowest temperature
2 K, however, there appear several weak
Bragg peaks [see arrows in Fig. 1(b)]; since
this temperature is well below TN , they are
most likely the magnetic Bragg peaks associated to the macroscopically observed
antiferromagnetic ordering. Magnetic aswell as crystallographic structure analysis
is now in progress using homemade Rietveld analysis code with the group theoretical representation analysis for the magnetic structure determination [2].
References:[1] B. K. Lee et al., Phys. Rev. B 70 (2004)
224409.
[2] I. Nakanowatari et al., Phys. Rev. B 76
(2007) 184427.

Intensity (counts)

Effect of geometrical frustration in the localized spin systems has been intensively
studied to date.
A number of novel
low-temperature phenomena have been reported there, exempliﬁed by the spin freezing, spin liquid and spin ice, to note a
few. Geometrical frustration may also
bring about non-trivial magnetic orderingin the metallic system at low temperatures. In particular, competition/interplay
between the strong electron correlations
and geometrical frustration is an intriguing
issue to study.
The ternary compound Ce5 Ni2 Si3 crystallizes in the hexagonal Ce2 NiSi-type
structure with the space group P63 /m. The
Ce Atoms are at the corners of trigonal
prisms, forming a locally triangular lattice
net [1]. The linear Sommerfeld coefﬁcient γ
is about 300 mJ/Ce mol K2 , which is a signof heavy fermion formation in this compound. An antiferromagnetic order wasobserved at TN = 7.3 K, whereas the Weisstemperature θ = −61.3 K, resulting in thefrustration index f ∼ 8. Although macroscopic magnetic properties have been reported to a large extent, spin structure in
the ordered phase has not been determinedyet.
In this study, we performed the powder
neutron diffraction experiments to determine the crystal as well as the spin structure at low temperatures in Ce5 Ni2 Si3 . The
experiments have been performed at IMRHERMES powder diffractometer. A powdered sample (about 4 grams) was loadedin the vanadium cell with the diameter of
7 mm, and then attached to the closed cycle refrigerator. The powder diffractgrams
were recorded at 2 K, 15 K, and 300 K.
Figure 1 shows the resulting powder
diffraction patterns at the low tempera-

60000
(a)
50000
40000
30000
20000
10000
0
0
8000
(b)
7000

T = 2KT = 15K
Ce5Ni2Si3 Powder HERMES

20

40

60

80

100

120

140

160

35

40

45

6000
5000
4000
3000
2000
0

5

10

15
20
25
30
Two theta (deg.)

Fig. 1. Neutron powder diffraction patterns at
T = 2 K (red) and 15 K (blue) measured at IMRHERMES.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 639

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JAEA-Review 2011-050

1-2-44

Studies of a quadrupolar ordering and magnetic excitations in YbAs
A. Oyamada, K. Kuwahara, K. Iwasa, K. Ohoyama and M. Kohgi
Kyoto Univ. , Tokyo Metropolitan Univ., Tohoku Univ.
YbAs is a possible candidate of aquadrupolar ordering system at hightemperature (80 K). It was reported by
ETH group that the ﬁrst excitation levelof crystal ﬁeld splitting (Gamma8) is split
below 80 K. This splitting was attributed
to a quadrupolar ordering.
In order to investigate the splitting ofGamma8 state, we observed the Gamma6Gamma8 excitation of YbAs by inelastic
neutron scatterings.
We found a Gamma6-Gamma8 splitting below 80 K.
The splitting has temperature dependence
which conﬁrms the previous data reported
by ETH group.
Furthermore we found that the phonon
spectra does not change at 80 K.
These results suggest that a transition at 80
K is a quadrupolar one.
Further experiments on q-dependence are
required.

Intensity (Counts / 5 min)1200
~ 17 K

1000
800
600
400
200
0

5

10

15

20

25

30

35

Energy (meV)Fig. 1. Energy spectra of YbAs at 17 K.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 659

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JAEA-Review 2011-050

1-2-45Magnetic property of Ag-In-Tb 1/1 approximant and its relation to Zn-Mg-RE
quasicrystals
S. Ibuka, K. Iida and T. J. Sato
ISSP-NSL Univ. Tokyo,
Quasicrystals are characterized by sharp
Bragg reﬂections with a point symmetry
which is forbidden in a periodic lattice,such as the ﬁve-fold symmetry. For magnetic quasicrystals, non-trivial spin ordering arranged on a quasiperiodic lattice is
expected theoretically. But up to now thelong-range order has not been observedin any magnetic quasicrystals. Even ZnMg-RE(RE=rare earth) quasicrystals whichhave well localized and large 4f magnetic
moments just indicate spin-glass-like transition or no transition[1]. The absence ofthe long-range order evokes a new question whether quasiperiodicity is essentially
incompatible with the long-range magnetic
order or not.
An approximant is a periodic crystal thathas a similar or identical atomic cluster ina ﬁnite length scale. Therefore, by studying magnetism of the approximants, one
may separately elucidate the effect of thelong-range quasiperiodicity and that of theshort-range clusters. Fortunately, a magnetic approximant to the icosahedral quasicrystal has been found in Ag-In-RE systems. They seem to have well localized moments as is the case in Zn-Mg-RE, and are
more suitable for neutron scattering than
Cd-RE approximants in terms of the absorption. Our measurement of static magnetization of Ag-In-Tb 1/1 approximant
showed that it has a spin-glass-like transition at T = 3.7 K, which is similar to that of
Zn-Mg-Tb at 5.8 K[1]. To elucidate difference from Zn-Mg-RE quasicrystals in magnetic ordering, we have performed neutron
powder diffraction study at 4G-GPTAS and
T1-3-HERMES.
The sample was prepared by melting
constituent elements and by annealing theresultant as-cast alloy in an appropriatemanner. The data shown in Figure 1 aretaken with incident energy Ei = 13.7
meV in the double-axis mode.
Theyshow clear nuclear Bragg reﬂections, which
are independent of temperature; no magnetic Bragg reﬂection was observed at thelowest temperature. we also conﬁrmed
the absence of the magnetic Bragg reﬂection using T1-3-HERMES. Figure 1 also
shows temperature difference of the powder diffraction patterns measured at 3.5 K
and 60 K. It clearly shows two broad peaks
at 0.6 and 1.9 Å−1 , indicating the development of the short-range-spin correlations
at low temperatures. This contrasts to thethree-peak feature of the magnetic diffuse
scattering pattern in Zn-Mg-Tb. The peak
at 0.6Å−1 develops below 40 K, which ismuch higher than the freezing temperature of 3.7 K. Further study using a single
crystalline sample is desired to elaborate
the short-range-spin correlations in the approximant.
[1] T. J. Sato, Acta Cryst. A61 (2005) 39.

Fig. 1. Neutron powder diffraction patterns at T =3.5 K(red) and 60 K(green) obtained at 4G-GPTAS.
Temperature difference [I(3.5 K) - I(60 K)] as a magnetic scattering contribution is also shown by theblue triangles.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 662

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JAEA-Review 2011-050

1-2-46
Crystal Structure and Magnetic Properties of CoZn(TeO3 )Br2
T. Kashi, Y. Yasui, T. Moyoshi, M. Sato, K. Kakurai1 , S. Iikubo1 , N. Igawa1
Department of Physics, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8602
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

CoZn(TeO3 )Br2 has been newly synthesized and its crystal and magnetic structures have been determined by powder neutron diﬀraction studies.1) T-Te-O-X systems(T=transition metals, X=Cl, Br) exhibit avariety of interesting magnetic properties. For
example, Co2 (TeO3 )Cl2 with the saw-toothlattice of Co2+ ions exhibits two successive
magnetic orderings at temperatures TN1 ∼73
K and TN2 ∼15 K.2) Another example
Co2 (TeO3 )Br2 has the linkage of Co(2)O4 Br2octahedra and Co(1)O2 Br2 tetrahedra, forming a two dimensional Co spins, which order at TN ∼29 K.3) Here, to add a newmember to the T-Te-O-X systems, we havesynthesized CoZn(TeO3 )Br2 . This new system has been found to be isomorphic to
Co2 (TeO3 )Br2 by neutron structural analysis
and can be derived by the total substitutionof Co(1) sites with Zn atoms. Because theZn atoms decouple the magnetic interaction
among the chains of Co(2) moments of thecorner-sharing Co(2)O4 Br2 octahedra, inducing the one-dimensionality of Co spins, themagnetic characteristics of the new system isquite diﬀerent from that of Co2 (TeO3 )Br2 . It
is interesting to study what magnetic characteristics are observed for this new Co2+ one
dimensional spin system. We have carriedout measurements of the magnetic susceptibility χ and speciﬁc heat C. Neutron magnetic structure analysis has also been carriedout in parallel with the neutron crystal structure analysis. The powder neutron diﬀraction studies have been carried out at the highresolution powder diﬀractometer (HRPD) of
JRR-3 of JAEA in Tokai. Rietveld analyses
were carried out by using the computer program Rietan 2000.

C/T -T curve.
The magnetic structure below TN has been
determined by a powder neutron diﬀraction
study, where Co spins within a chain arefound to order basically in an antiferromagnetic way with the spins along the c direction(chain direction), but they are canted fromthe c-axis toward the b-axis by an angle of 17(±3) ◦ . The ordered moment is 1.78(±0.03)
μB . To explain the ferromagnetic magnetization of the powder samples (∼0.024 μB ),the spins should have another canting possibly toward the a-axis at an angle of 7.9◦ . Then, for the understanding of the noncollinear and complicated magnetic structure of CoZn(TeO3 )Br2 , we should consider
the competition of eﬀects originating fromthe single ion anisotropy and DzyaloshinskiMoriya interaction, for example. The existence of the T -linear component of the speciﬁc heat has been reproducibly observed. We
note that the ordered moment at T =3 K is
1.78 μB , much smaller than the value of 3 μB
usually expected for the high spin state Co2+
state. These results suggest that a signiﬁcant
fraction of Co spins remains in the disorderedor glassy state.
References
1) T. Kashi et al.; J. Phys. Soc. Jpn. 77 (2008) 084707.
2) T. Kashi et al.; J. Phys. Soc. Jpn. 76 (2007) 084713.
3) R. Becker et al.; J. Solid. State. Chem. 179 (2006)
836.

A transition to an antiferromagnetic stateaccompanied by the weak ferromagnetic moment has been observed at the Neel temperature TN =9.0 K. The Weiss temperature θW
is estimated to be ∼68.5 K from the magnetic susceptibility data. The absolute ratioof the Neel and Weiss temperatures |TN /θW |is ∼0.13. A broad peak at TN exists in the
原子炉：JRR-3

装置：HRPD(1G)

㫦
㫦

F

D

E

&R

Figure 1: Magnetic structure of CoZn(TeO3 )Br2 .

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JAEA-Review 2011-050

1-2-47
Linear Relation between Electric Polarization and Magnetic Chirality in theCommensurate Phase of RMn2 O5 (R =Ho, Er)
S. Wakimoto, H. Kimura1 , M. Fukunaga1 , K. Nishihata1 , M. Takeda, K. Kakurai, Y. Noda1 ,and Y. Tokura2
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577
2
Department of Applied Physics, University of Tokyo, Tokyo 113-8656

Multiferroic materials RMn2 O5 (R: rareearth) show antiferromagnetic order and ferroelectricity concomitantly at low temperatures with strong coupling, resulting in a remarkable magnetoelectric eﬀect 1, 2) . The understanding of the coupling mechanism is oneof the central issues.
To date, two distinct models have been suggested as an origin of the magnetoelectric coupling in the Mn multiferroics. One is an inverse Dzialoshinski-Moriya (DM) interaction
model 3) and the other is called exchange
striction model 4) . The former produces polarization from a cross term of spins Si × Sj ,while the latter based on Si · Sj products.
Recently, it is shown that the commensurate(CM) magnetic structure of the ferroelectricphase of RMn2 O5 (R=Y, Er, Ho) contains
spirals of the Mn spins with magnetic unit cellof (2a, b, 4c) 5) , which create the polarization
based on the inverse DM mode. Therefore,
the role of the magnetic spiral in the magnetoelectric coupling is of great interest. Here
we report results of polarized neutron scattering experiments under electric ﬁeld in the CMphase of HoMn2 O5 and ErMn2 O5 .
Polarized neutron scattering experiments
were done at TAS-1. A combination of a pyrolytic graphite (PG) monochromator and a
Heusler analyzer has been used with a spin
ﬂipper in front of the analyzer. A guide ﬁeld
around the sample was kept either parallel tothe momentum transfer Q (horizontal ﬁeld)
or vertical by a Helmholtz coil. The incident
neutron energy Ei = 14.7 meV and the collimator sequence of 40 -80 -80 -open were used.
PG and sapphire ﬁlters were located in frontof the sample to eliminate higher order andfast neutrons, respectively. In this conﬁgura原子炉：JRR-3

装置：TAS-1(2G)

tion, we can analyze the polarization of thediﬀracted neutrons where the incident beam
is unpolarized.
Disk-shaped single crystals of RMn2 O5(R =Ho, Er) with a thickness of ∼ 1 mmalong the b-axis were placed in a closed-cycle
He-gas refrigerator. The b-axis was set vertical, so that one can access to (H, 0, L) typereﬂection. Electrodes were attached on gold
masks on the b-surface. In the measurements,
we cooled the sample from 65 K to 20 (23) K
for R =Er (Ho) under electric ﬁelds up to
1 kV, then measure neutron scattering followed by a warming procedure without ﬁeld.
In warming, pyrocurrent has been measured
to evaluate the electric polarization.
The polarization of the incident anddiﬀracted neutrons, Pi and Pf , are connectedby the following formula in the magnetic scattering cross section from a magnetic structurewith chirality:
Pf σ = {−Pi +2(Pi · M̂)· M̂}·σm +i(M×M∗ ),
(1)
where


Sj⊥ cos Q · rj + i
Sj⊥ sin Q · rj .
M=
j

j

(2)
Here, σm is the magnetic cross-section without chirality, Sj⊥ is a component of the j−thspin perpendicular to Q. The ﬁrst term in
Eq. (1) means that the neutron polarization makes π-precession with respect to M.
The second term expresses the chiral structure contribution indicating that the ﬁnal polarization is forced to align along the chiral
vector i(M × M∗ )//Q. In our experimental set-up, therefore, the diﬀerence in the spin(+) and (-), (σ+ − σ− ) ∝ Pf , in the horizon-

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JAEA-Review 2011-050

tal ﬁeld mode observes the magnetic chirality
directly.
Figures 1 (a) and (b) show magnetic chirality in the CM phase of HoMn2 O5 andErMn2 O5, respectively, as a function of theelectric polarization of the bulk sample along
the b-axis. The data at ∼ 5 nC for Fig.
1 (a) and those for ∼ 2 nC for Fig. 1(b) are measured after cooling under a zeroﬁeld, while the others are either data measured after cooling in ±1 kV. We note that
our samples show spontaneous polarization
after the zero-ﬁeld-cooling. This is becauseof a sample-dependent peculiarity that polarized domains are imbalanced even after
the zero-ﬁeld-cooling process 6) . The chirality has been measured at both Q-positions
near the a∗ -axis, (1.5, 0, ±0.25) for HoMn2 O5and (2.5, 0, ±0.25) for ErMn2 O5 , and near
the c∗ -axis, (0.5, 0, ±1.75) for HoMn2 O5 and(0.5, 0, ±2.25) for ErMn2 O5 . Since the neutrons see magnetic component that is perpendicular to Q, the former corresponds tothe magnetic chirality in the bc-plane while
the latter in the ab-plane. For both samples, particularly for HoMn2 O5 , it is demonstrated that the chirality is proportional tothe electric polarization even with the zero30

1) T. Kimura et al., Nature 426, 55 (2003).
2) N. Hur et al., Nature 429, 392 (2004).
3) H. Katsura, N. Nagaosa, and A. V. Balatsky, Phys.
Rev. Lett.95, 057205 (2004).
4) L. C. Chapon et al., Phys. Rev. Lett.96, 097601(2006).
5) H. Kimura et al., J. Phys. Soc. Jpn.76, 074706(2007).
6) M. Fukunaga et al.,J. Korean Phys. Soc. 51,
768 (2007).
7) Y. Yamasaki et al., Phys. Rev. Lett.98, 147204(2006).

30(a) HoMn2O5(b)

ErMn2O5

20

10
0
-10
-20
-30
-10

Referenceschirality (a.u.)chirality (a.u.)

20

ﬁeld-cooling data. Also we have conﬁrmedthat the high-temperature ICM phase, whichis paraelectric, does not show the chirality.
Thus, the magnetic chirality universally connected to the electric polarization for the CMphase of RMn2 O5 with R =Ho and Er, andthe ferroelectric phase of TbMnO3 7) However, there is an important question for theRMn2 O5 system why the large electric polarization achieves in the CM structure. To address this, detailed magnetic structure analyses for the high-temperature as well as lowtemperature ICM phase are necessary.

10
0
-10
-20

-5

0
P (nC)

5

10

-30
-10

-5

0
P (nC)

5

10

Figure 1: Chiral terms for (a) HoMn2 O5 and (b) ErMn2 O5 as a function of the electric polarization of bulk
crystal along the b-axis. The chirality is determined by σ+ − σ− . For HoMn2 O5, the chirality is measured at(1.5, 0, 0.25) (ﬁlled circles), (1.5, 0, −0.25) (open circles), (0.5, 0, 1.75) (ﬁlled squares), and (0.5, 0, −1.75) (opensquares). For ErMn2 O5 , it is measured at (2.5, 0, 0.25) (open circles), (2.5, 0, −0.25) (ﬁlled circles), (0.5, 0, 2.25)(open squares), and (0.5, 0, −2.25) (ﬁlled squares).

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JAEA-Review 2011-050

1-2-48Polarization of the Spin-Wave Modes in the Kagomé Lattice Antiferromagnet
KFe3 (OH)6 (SO4 )2K. Matan1 , J. S. Helton1 , D. Grohol2 , D. G. Nocera3 , S. Wakimoto4 , K. Kakurai4 , andY. S. Lee1
1

Department of Physics, Massachusetts Institute of Technology, Cambridge, MA USA
2
The Dow Chemical Company, Core R&D, Midland, MI 48674, USA
3
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
4
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Collective behavior in strongly correlated
systems often leads to unconventional groundstates. One example of such systems is geometrically frustrated spins, where the incompatibility between the topology of an underlying lattice and spin interactions prevents
the system to be in a unique ground state,
prompting the presence of novel spin dynamics. The kagomé lattice antiferromagnet is a highly frustrated two-dimensional lattice, being comprised of corner-sharing triangles. One of the hallmarks of this system is the “zero energy modes”, which result
from the highly degenerate, but connected,
ground state manifold. One ideal realization of the kagomé lattice antiferromagnet isjarosite KFe3 (OH)6 (SO4 )2 . Due to the presence of the Dzyaloshinskii-Moriya (DM) interaction in this material, the spins order in
a q = 0 structure with small canting forming
an “umbrella” spin conﬁguration below theNéel temperature TN = 65 K1, 2) . The DM
interaction also lifts the “zero energy mode”
to a ﬁnite energy, making it measurable byneutron scattering. We have previously reported on the ﬁrst observation of this liftedzero energy mode in jarosite, and determined
all relevant spin Hamiltonian parameters3) .
Inelastic polarized neutron scattering measurements were performed on TAS-1 spectrometer at Japan Atomic Energy Agency,
Tokai, Japan. This state-of-the-art instrument utilizes double-focusing Heussler crystals to monochromate and analyze the incident and scattered neutron beams. The
beam polarization of more than 90% isachieved.
The ﬁnal neutron energy was
ﬁxed at 14.7 meV. Horizontal collimations
原子炉：JRR-3

装置：TAS-1(2G)of open−80 −sample−open−open were employed. However, due to the small sample,
eﬀective horizontal collimations of 48 − 18 −sample − 25 − 240 were used to calculate theresolution function. Pyrolytic graphite ﬁlters
were placed in the scattered beam to reduce
higher-order contaminations. The energy resolution of about 1.2 meV and background of
about one count per minute were achieved. A
single crystal of jarosite of mass 48 mg wasoriented in the (HK0) zone. The sample wascooled by a 4 He close-cycle displex.
The spin-wave calculations of the spin
Hamiltonian show three branches of low energy spin excitations, which correspond totwo out-of-plane excitations and one in-plane
excitation4) . By choosing proper orientationsof a polarization vector P, which is deﬁned by
the direction of a guide ﬁeld, and wave vector
Q, one can distinguish between the in-planeand out-of-plane spin excitations. If P and
Q are parallel, both in-plane and out-of planemagnetic excitations will give rise to scattering intensity in the spin-ﬂip (SF) channel. On
the other hand, if P is perpendicular to Q,
then the magnetic scattering in the SF channel is due to the excitations that are perpendicular to both Q and P, and the magnetic
scattering in the non-spin-ﬂip (NSF) channel
is due to the excitations parallel to P.
Fig. 1 shows constant-Q scans at (1,0,0),
the center of the Brillouin zone (Γ−point),
measured at 10 K. The observed peaks were ﬁt
with narrow Gaussian convoluted with the experimental resolution function assuming theempirical dispersion3) . For the guide ﬁeld
along Q (HF) (Fig. 1(a)), both spin-wave excitations at 2 meV and 7 meV were observed

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JAEA-Review 2011-050

Figure 1: Inelastic polarized neutron scattering measurements of spin-wave excitations at the zone center.

in the SF channel, while there is no magnetic
scattering in the NSF channel. For the guideﬁeld perpendicular to Q, and perpendicular
to the scattering plane (VF) (Fig. 1(b)), thepeak at 2 meV was observed in the SF channel, and the peak at 7 meV was observed in
the NSF channel. On the other hand, if theguide ﬁeld was perpendicular to Q, but lay
within the scattering plane (HFy ) (Fig. 1(c)),
then the peak at 2 meV was observed in the
NSF channel and the peak at 7 meV was observed in the SF channel. The equivalent intensities in the VF SF (VF NSF) and HF SF(HF SF) channels and the absence of intensity
in the VF NSF (VF SF) channel at 2 meV (7meV) indicate that the 2 meV (7 meV) excitation is predominantly the in-plane (outof-plane) excitation, consistent with the spinwave analysis.
The polarization of the spin ﬂuctuations
were also studied using polarized neutron
scattering. Fig. 2 shows constant-Q scan at(1 0 0) through a quasi-elastic peak measured
at T = 67 K. The observed quasi-elastic peak
was ﬁt to Lorentzian convoluted with the experimental resolution function. Backgrounds
and peak widths were kept constant for alldata sets. The intensities in the HF SF and
VF SF channels indicate that the spin ﬂuctuations are predominantly the in-plane ﬂuc-

Figure 2: Quasi-elastic scattering centered at (1 0 0)
measured by polarized neutrons at 67 K.

tuations, providing the direct evidence forthe presence of XY symmetry previously reported in Ref. 2.
In jarosite, the spin gaps are a result of theantisymmetric DM interaction. To the leading order, the analytic expressions show thatthe in-plane gap is proportional to |Dp | whilethegaps are proportional to√ two3,out-of-plane
J1 Dz 4) . Therefore, despite the similar Dp
and Dz , the out-of-plane gap is signiﬁcantly
larger than the in-plane gap. Above TN only
the in-plane rotational (XY ) symmetry is restored. This result immediately suggests theexistence of the out-of-plane gap above TN . In
fact, our polarized neutron scattering aroundthe quasi-elastic peak above TN exhibits thein-plane-only spin ﬂuctuations, which imply
that the out-of-plane gap remains at a ﬁnite energy. Therefore, in the critical regime,
KFe3 (OH)6 (SO4 )2 , whose interlayer couplingis negligibly small1) , is a promising candidate
for studying the 2D XY universality class inmagnetic systems.
References
1) D. Grohol et al., Nature Mater. 4 (2005) 323.
2) T. Inami et al., Phys. Rev. B 61 (2000) 12181.
3) K. Matan et al., Phys. Rev. Lett. 96 (24) (2006)
247201.
4) T. Yildirim, A. B. Harris, Phys. Rev. B 73 (21)(2006) 214446.
1-2-48㻙㻌 㻝㻡㻞㻌㻙

JAEA-Review 2011-050

1-2-49Investigation of in-plane Magnetic Structure in NpFeGa5
T. Sugai1,2 , F. Mizuno1,2 , K. Kaneko1 and N. Metoki1,2
Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195
2
Department of Physics, Tohoku University , Sendai 980-8578

NpTGa5 (T=Fe, Co, Ni, Rh and Pt) is an
isostructual family of heavy fermion superconductors CeT Ga5 and PuT Ga5 . The magnetic structures of NpT Ga5 were studied byour recent systematic neutron scattering experiments. We found the variety of the magnetic structures and double transitions, which
can be understood in terms of a localized
model. For example, our neutron polarization analysis revealed that NpFeGa5 shows
C-type AFM with magnetic moment parallel to the 110 direction, while below 78K,
magnetic moment rotates to c-axis at the angle 25◦ . Kiss et al. 1) explained this unusual
magnetic moment direction with quadrupoleorder parameter Ozx , which induces both inplane(μc-axis) and out-of-plane(μ⊥c-axis)
dipole moment. Furthermore S. Kambe etal. 2) proposed that magnetic moment slightly
rotate, i.e. μ [110]+[11̄0], from the splittingof NMR spectra at Ga site, due to mixing of
small Ozx  and large Oyz . Neutron spinpolarization analysis of single domain sample
of NpFeGa5 with application of vertical magnenic feld has been carried out in order toreveal this additional in-plane component.
Neutron scattering experiments have been
carried out using triple-axis spectrometer
TAS-1 installed at the research reactor JRR3 at the Japan Atomic Energy Agency. The
sample dimension was 1.75×1.75×1.25 mm3 .
We studied (1/2 1/2 0) AFM Bragg scattering from single domain sample with the [hhl ]scattering plane(stabilized via vertical magnetic ﬁeld along [11̄0]). With this conﬁgration, non spin ﬂip(NSF) cross section detects
vertical component perpendiculer to the scattering plane, while spin ﬂip(SF) component
is proportional to the squared moment along
the c-axis.
Fig.2 shows the NSF cross section signalof the (1/2 1/2 0) at 1.5 K. We observed a
原子炉：JRR-3

装置：TAS-1(2G)very weak scattering intensity above the background level. After correcting depolarization
obtained by ﬂipping ratio, we concluded thata possible magnetic moment of about <0.1
μB . This small moment would be consistent with small splitting in NMR study by S.
Kambe et al.. In order to get the ﬁnal conclusion about the existence of the small in-planecomponent, we need to improve signal statics.
[Figure]c

T < 78Ka78K < T < 118K

Figure 1: Magnetic structure of NpFeGa5 .

Intensity (Counts/1200sec)

1

350(0.5 0.5 0)
5T
1.5K
Non Spin Flip

340
330
320
310

BG

300
290
280
-14

-12

-10

ω

 -8-6

Figure 2: Non Spin ﬂip(NFS) scattering at (1/2 1/20) . The broken line indicates back ground.

References
1) A. Kiss et al. :“J. Phys. Soc. Jpn.”, 75, 034709(2006).
2) S. Kambe et al. :“Phys. Rev. B”, 76, 144433(2007).

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JAEA-Review 2011-050

1-2-50Unusual ﬁeld-induced Antiferromagnetic Order in NpIn3
F. Mizuno1,2 , T. Sugai1,2 , N. Metoki1,2 and K. Kaneko2
1

Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195
2
Department of Physics, Tohoku University , Sendai 980-8578

Very recently we have systematicallyrevealed the magnetic structure of NpTGa5
which is an iso-structural family of havy
fermion superconductors CeTGa5 and
PuTGa5 . We reported possible quadrupoleorder in many body itinerant 5f electron
system. NpTGa5 has layered structure withsequential stacking of NpGa3 and TGa2layers.
Thus our study recalls renewedinterests in NpX3 mother crystal with AuCu3
structure. The triplet state under cubic
symmetry provides a more suitable situation
for the orbital degree-of-freedom as a possible origin of the multiple phase diagram,
successive transition and meta-magnetic
behavior. We have studied the magnetic
structure and the magnetic phase diagram of
NpIn3 systematically under horizontal andvertical magnetic ﬁeld with use of neutron
spin polarization technique.

ment parallel to the ﬁeld direction as shownin Figures. The direction of the AFM modulation was also conﬁrmed by the neutron spinpolarization analysis.
AFM modulation in spin ﬂip phase is perpendicular to the external ﬁeld as a resultof the energy gain from induced moment byexternal ﬁeld, where there is a slight energy
loss of exchange energy due to small tiltingof the AFM moment. A similar structure has
been reported in the ﬁeld induced phase of
PrOs4 Sb12 , where the quadrupole order appears for high ﬁeld [3]. Therefore this unusual
structure would be a signature of ﬁeld induced
quadrupole order in NpIn3 .
[Figure]500

原子炉：JRR-3

装置：TAS-1(2G)(a) (-1/2 1/2 0)
T = 1.6 K
H=0T
5T

14
2

15
16
(b) (-1/2 1/2 0)( deg.
) K
T = 1.6

400
Intensity ( cnt / 600 s )For H =0 we observed ferromagnetic (FM)scattering at (001) for TN < T < TC , and antiferromagnetic (AFM) modulation with q =(3/8 3/8 3/8) at the ground state for T < TN ,which is consistent with a previous study 1) .
We observed a sharp transition between FM
and AFM structure. No coexistence of both
FM and AFM has been observed.
We observed that the AFM peak disappeared with application of magnetic ﬁeld
H =5 T along [110]. We found (1/2 1/2 0)
AFM modulation accompanied by the metamagnetic phase. Surprisingly, we found that
the AFM modulation amplitude is parallelto the ﬁeld direction. Namely Np subllatice
has two diﬀerent size of Np magnetic moment
which is parallel to the external ﬁeld. This isrevealed by the horizontal ﬁeld experimentswith H //[110] applied on the [hk0] scattering
plane. The AFM reﬂection at Q=(1/2 -1/2 0)
for Q ⊥ H, while no peak observed at (1/2 1/20) with Q // H, indicative of the AFM mo-

NpIn3

300
200
500

13

H=0T
5T

400
300
200
13

14
2


15
( deg. )16

Figure 1: Field induced antiferromagnetic reﬂection of
NpIn3 for (a) Q ⊥ H and (b) Q//H, respectively.

References
1) E. Colineau : Ph.D. Thesis.
2) D. Aoki etal. :“J. Phys. Soc. Jpn”, 75, 084710(2006).
3) K. Kaneko etal. :“Phys. Rev. B”, 75, 094408(2007).

分野：中性子散乱（磁性）㻙㻌 㻝㻡㻠㻌㻙

JAEA-Review 2011-050

1-2-51

Magnetic Structure of LiCu2 O2
Y. Yasui, K. Sato, T. Moyoshi, M. Sato, K. Kakurai1

Department of Physics, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8602
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Materials with magnetic and ferroelectric
coexisting orders are called multiferroics andattract much attention. While almost all multiferroic systems ever reported have the magnetic moments with spin S ≥ 1 and/or havemore than two magnetic sites, the authors’group have found that LiVCuO4 is a multiferroic with Cu2+ spins S=1/2 in the 3d, x2 y 2 orbital and only one crystallographicallydistinct Cu site.1,2) To understand the multiferroic nature, studies of the spin 1/2 multiferroic systems are very useful, because there
are not any complications due to the multiorbital and multi-site eﬀects. LiCu2 O2 withsimilar structural characteristics to those of
LiVCuO4 , but with two crystallographicallydistinct Cu sites has also been reported to
be multiferroic.3) However, we think that certain problems remain on the reported multiferroic behavior3) and magnetic structure4) of
LiCu2 O2 , because an inconsistency exists in
the relationship between the magnetic structure and observed ferroelectiric polarization.
Moreover, the ab-helical magnetic structurereported in ref. 4 cannot explain the 7 LiNMR spectra obtained by our group. (Dueto the existence of the double CuO2 ribbon
chains shown in the inset of Fig. 1 makes it
diﬃcult to determine the magnetic structureof LiCu2 O2 .)Neutron scattering studies have been carried out on single crystals using the triple
axis spectrometer TAS-1 installed at JRR-3
of JAEA in Tokai. To avoid the large neutron absorption of Li, we used 7 Li isotope in
the growth of crystals. The neutron scattering intensities were measured at Q=(h, k, 0)and (h, k, 2h) in the reciprocal space at 3.2 K(< TN ∼22.5 K) and 50 K (> TN ). At 3.2 K,
we observed magnetic superlattice reﬂections
at Q=(h, k ± δ, 0) and (h, k ± δ, 2h) (h=halfinteger and k=integer) with δ ∼0.172. Figure
1 shows the temperature dependence of theintegrated intensity of 1/2 δ 1 magnetic reﬂection. From the ﬁgure, the magnetic ordering is found to grow with decreasing T below
TN . The Cu2+ spins have incommensurate
原子炉：JRR-3

装置：TAS-1(2G)

magnetic structure with modulation vector ofδb∗ (or the pitch angle along the CuO2 ribbon chains is ∼62◦ ). First, we analyzed theobtained magnetic scattering intensities at 3.2
K by using the initial spin directions and angles of four chains in the unit cell as the parameters, assuming that the magnetic structure is sinusoidal or helical type. We foundthat the observed scattering intensities cannot be reproduced by the magnetic structuresdescribed by varying the above parameters.
(Note that the ab-plane helical structure reported in ref. 4 can be obtained by varying
the above parameters.) At 3.2 K the magnetic structure is, we think, very complicatedand spins have nonzero components in all of
the three directions. Detailed magnetic structure analysis is being carried out by adopting
other possible models.
References
1) Y. Naito et al.; J. Phys. Soc. Jpn. 76 (2007) 023708.
2) Y. Yasui et al.; J. Phys. Soc. Jpn. 77 (2008) 023712.
3) S. Park et al.; Phys. Rev. Lett. 98 (2007) 057601.
4) T. Masuda et al.; Phys. Rev. Lett. 92 (2004) 177201.

Figure 1: T -dependence of scattering intensity for 1/2
δ 1 (δ ∼0.172) reﬂection. Inset shows the schematic
structure of LiCu2 O2 .

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JAEA-Review 2011-050

1-2-52
Investigation of the Giant Magnetic Moments in Nitrogen-Martensites thin
Films Using the Polarized Neutron Diﬀraction Technique
M. Takeda1,2,3 , K. Kakurai1 , K. Sunaga4 ,M. Tsunoda4 , M. Takahashi41

Quantum Beam Science Directorate, Japan Atomic Energy Agency,
Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan
2
J-PARC Center, Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan3
New Industry Creation Hatchery Center, Tohoku Univ., Aramaki Aoba,
Aoba-ku, Sendai-shi, Miyagi, 980-8579, Japan
4
Graduate School of Engineering, Tohoku Univ., Aramaki Aoba,
Aoba-ku, Sendai-shi, Miyagi, 980-8579, Japan

External magnetic fields

α"– Fe 16 N2 [110] //Mg O[010]

Q
[001]

α"– Fe 16 N2 [110] //Mg O[100]装置：TAS-1(2G)

MgO(002)

Si(004)

MgO(004)(001)
NSF 10kOe
SF 10kOe
NSF 630Oe
SF 630Oe
FR 10kOe
FR 630Oe

7
6
5
4
3

1.5

2

105
1.0

7
6
5
4

MgO(001)

MgO(003)

Si(002)

3
2

0.5
4

MgO(005)
Si(006)
(008)

10

(004)

7
6
5
4

(002)

3

0.0
0

10

20

30

40

50

-1

60

70

80

90

100

Q (nm )

Figure 2: Polarized neutron diﬀraction intensities andﬂipping ratios. Scans were done along the [00l].

We determined the magnetic moments of Fe
on three diﬀerent sites in the unit cell as 2.19
(Fe I), 2.08 (Fe II), and 2.55 μB (Fe III) fromanalysis of the data in Fig. 2 and another datawith scans along [hh0]. There is no evidenceof the giant magnetic moments of the Fe16 N2
ﬁlms.
References

Figure 1: Epitaxial relations (left) and schematic representation of an assemble of 15 ﬁlms (right).

原子炉：JRR-3

2.0

2

6

10

Counts / 60 sec.

The samples were prepared by the reactivity sputtering with N2 gas on MgO substrates.
15 pieces of the ﬁlms were glued on a plate of
the single crystal of Si so as to align the [001]and [11̄0] axes of Fe16 N2 of the ﬁlms (Fig. 1).
The diameter of each ﬁlms is 5 mm φ, andthe thickness of the ﬁlms 300 nm. The ﬁlms
have a buﬀer layer of Fe with the thickness of
5 nm, and a cap layer of Cu with 50 nm.

An external magnetic ﬁeld of 10 kOe wasapplied to the sample to saturate the Fe magnetization in the ﬁlms. The neutron energy was ﬁxed at 14.7 and 80 meV( λ =0.237 and 0.098 nm) by a Cu2 MnAl polarizing monochromator. Neutron spin was set toparallel or antilarallel to the magnetization of
the sample using a spin-ﬂipper set before thesample. Each intensity with the spin-ﬂipper
oﬀ (I+ ) and with on (I− ) was independently
counted, and then a ﬂipping ratio (I+ /I− ) was
obtained (Fig. 2).

flipping ratio

Since the discovery of a giant magnetic moment of 2.9 T in Fe16 N2 thin ﬁlms by Kim etal., a lot of research have been done to try toshow clear evidence of the giant magnetic moments. It has been, however, enable to conclude because of inhomogeneity of the sample. The Fe16 N2 ﬁlms consists of α and α”
phases of Fe16 N2 , but it was diﬃcult to control the ratio. Takahashi et al. have successfully synthesized the (α + α”)−Fe16 N2 ﬁlms,
and have performed magnetization measurements, Mössbauer spectroscopy and so on2) .
They did not ﬁnd out the giant magnetic moment in their ﬁlms. We performed the polarized neutron diﬀraction measurements of the
Fe16 N2 ﬁlms to give the ﬁnal conclusion.

1) T. K. Kim and M. Takahashi, Appl. Phys.Lett.,
20, 492 (1972).
2) H. Takahashi, H. Shoji, and M. Takahashi, J.
Magn. Magn. Mater., 174, 57 (1997).

分野：中性子散乱（磁性）㻙㻌 㻝㻡㻢㻌㻙

JAEA-Review 2011-050

1-2-53
Partial Disordered Phase of RbCoBr3
Y. Nishiwaki, A. Oosawa1 , K. Kakurai2 and T. Kato3
Department of Physics, Tokyo Women’s Medical University, Shinjuku-ku, Tokyo 162-8666
1
Department of Physics, Sophia University, Chiyoda-ku, Tokyo 102-8554
2
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
3
Faculty of Education, Chiba University, Inage-ku, Chiba 273-8522

The temperature dependence of the ( 13 13 1),
2 2( 3 3 1), and (1 1 1) neutron diﬀraction peakheights is shown in Fig. 1. The ( 23 23 1) peakis observed below 37.2 K but the (1 1 1) peakis observed only below 30.5 K. When the spin
structure is PD, the (1 1 1) peak disappears
and the ( 23 23 1) peak appears. Therefore, theintermediate PD phase is exhibited between
TN1 = 37.2 K and TN2 = 30.5 K.
Compared with the results of CsCoCl3 and
CsCoBr3 ,2, 3) , the temperature dependence ofthe (1 1 1) peak of RbCoBr3 exhibits analmost linear increase below TN2 with decreasing temperature. The results can be
原子炉：JRR-3

装置：TAS-2(T2-4)

explained by considering a lattice distortionaﬀecting the spin system. We considered
the spin-lattice model and performed Monte
Carlo simulations.4) In the model, the updown shifts of -CoBr3 - chains are represented
using the pseudospin variable. The pseudospin system has frustration in the same way
as the real-spin system. The exchange interactions between real spins depend on thepseudospin of the lattice variables. Detailsof the model Hamiltonian and analysis arereported elsewhere.4) As a result, the linear
temperature dependence of the (1 1 1) peakis well reproduced by the spin-lattice model,
as shown in Fig. 1.
35x10

3

RbCoBr3(2/3 2/3 1)

30
Neutron Counts [/80s]

RbCoBr3 realizes the distorted triangularlattice antiferromagnet with the Ising spin
system.1) . The crystal structure is distorted
through structural phase transitions from theCsNiCl3 structure. The lattice distortionis characterized by -CoBr3 - chain shift andthe geometrical frustration is released partially. The antiferromagnetic phase transition of RbCoBr3 was identiﬁed at TN =37.2 K, which agrees with the ferroelectrictransition temperature TC = TN . A previous neutron diﬀraction study reported that a
partial disordered (PD) phase was absent in
RbCoBr3 .1) The PD phase was found to appear on CsCoCl3 and CsCoBr3 , which havea nondistorted triangular lattice, at temperatures between the ground-state ferrimagnetic
phase and the paramagnetic phase.2, 3) In the
PD phase, one of the three sublattices is disordered and the other sublattices are aligned
antiferromagnetically. However, recent theoretical and experimental studies indicate that
RbCoBr3 should undergoes successive magnetic and structural phase transitions. Therefore, we reexamine the existence of the PD
phase.

25
20
TN1
15

(1/3 1/3 1)

10
TN2
5

(1 1 1)

0
0

10

20
Temperature [K]30

40

Figure 1: Temperature dependence of (1 1 1), ( 13 31 1),
and ( 23 32 1) neutron diﬀraction peak heights. The
numerical results of the model simulations are shownby lines.

References
1) Y. Nishiwaki, T. Kato, Y. Oohara, and K. Iio: J.
Phys. Soc. Jpn. 73 (2004) 2841.
2) M. Mekata: J. Phys. Soc. Jpn. 42 (1977) 76.
3) W. B. Yelon, D. E. Cox, and M. Eibschütz: Phys.
Rev. B 12 (1975) 5007.
4) T. Nakamura and Y. Nishiwaki: cond-mat/0803.1710.

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JAEA-Review 2011-050

1-2-54
Neutron Diﬀraction Study on Spinel GeCo2 O4 under Magnetic Field
M. Matsuda, T. Hoshi1,2 , H. Aruga Katori2 , M. Kosaka1 and H. Takagi2
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Graduate School of Science and Engineering, Saitama University, Saitama, Saitama 338-8570
2
RIKEN, Wako, Saitama, 351-0198

The spinel GeCo2 O4 has the pyrochlore lattice of Co2+ ions, in which the kagomé and triangular planes stack alternatively along the(111) direction. It shows an antiferromagnetic ordering with a characteristic wave vector of Q=(1/2, 1/2, 1/2) below TN ∼ 21
K 1) accompanied by a structural phase transition from cubic to tetragonal symmetry. 2)
The spin arrangement is ferromagnetic in the
kagomé and triangular planes and antiferromagnetic between the kagomé and triangular planes. 3) Recently, magnetic properties of
GeCo2 O4 in magnetic ﬁeld were studied. 2) It
was reported that GeCo2 O4 exhibits a magnetic phase transition at Hc ∼4 T when theﬁeld is applied along the (110) and (111) directions. The magnetic transition is probably
related with the frustrating interactions.

intensity probably originates from the combined eﬀects of the redistribution of the magnetic domains and a magnetic phase transition. We need more experiments using asingle crystal to distinguish the two eﬀects
and clarify the detailed magnetic structure inmagnetic ﬁeld.

In order to clarify the magnetic structure in magnetic ﬁeld, we performed neutron
diﬀraction experiments using a powder sample of GeCo2 O4 . The experiments were performed on the triple-axis spectrometer TAS-2
at JRR-3 at JAEA. Vertical magnetic ﬁeld
was applied up to 10 T using a new type of
split-pair superconducting magnet that uses
cryocoolers.
Magnetic ﬁeld dependence of some magnetic Bragg peak intensities was measured.
For example, the (1/2, 1/2, 1/2) Bragg intensity increases with increasing magnetic ﬁeld
up to 4 T and gradually decreases above 4 T
as shown in Fig. 1(a). This characteristic ﬁeld(∼4 T) is consistent with Hc determined fromthe magnetization measurments. 2) Furthermore, the hysteresis behavior was observed
between 0 and 4 T at 4 K. It becomes lessdistinct at 15 K as shown in Fig. 1(b). Thisbehavior probably originates from a reorientation of the magnetic domains in magnetic
ﬁeld. Therefore, the ﬁeld dependence of the
原子炉：JRR-3

装置：TAS-2(T2-4)

Figure 1: Magnetic ﬁeld dependence of the (1/2, 1/2,
1/2) magnetic Bragg intensity measured at T =4 K (a)and 15 K (b).

References
1) J. Hubsch and G. Gavoille: ”J. Magnetism Magnet. Mater.”, 66, pp. 17-22 (1987).
2) T. Hoshi, H. Aruga Katori, M. Kosaka and H.
Takagi: ”J. Magnetism Magnet. Mater.”, 310, pp.
e448-e450 (2007).
3) S. Diaz, S. de Brion, G. Chouteau, B. Canals, V.
Simonet and P. Strobel: ”Phys. Rev. B”, 74, pp.
092404/1-4 (2006).

分野：中性子散乱（磁性）㻙㻌 㻝㻡㻤㻌㻙

JAEA-Review 2011-050

1-2-55Magnetic Excitation in the Spin-1/2 Antiferromagnetic Alternating Chain
Compound β-AgCuPO4
M. Hase, M. Matsuda1 , K. Kakurai1 , K. Ozawa, H. Kitazawa,
N. Tsujii, A. Dönni and H. Kuore2
1

National Institute for Materials Science (NIMS), 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047
Japan Atomic Energy Agency (JAEA), 2-4 Shirakata Shirane, Tokai, Naka, Ibaraki 319-1195
2
Department of Physics, Sophia University, 7-1 Kioi-cho, Chiyoda, Tokyo 102-8854

The calculated results based on spin-dimer
analysis indicate that an exchange interaction
in a Cu-Cu bond with a long distance (5.20 Å)is the strongest (the J4 interaction in Fig. 7of Ref. 1) in insulating β-AgCuPO4 , although
there are short Cu-Cu bonds (3.10 and 3.20
Å). The J1 interaction in the same ﬁgure is thesecond strongest: the ratio J1 /J4 is 0.17. The
two interactions form an antiferromagnetic(AF) alternating chain. Actually, the magnetic susceptibility of β-AgCuPO4 shows theexistence of a spin-singlet ground state with aspin gap.1) Because we usually speculate thatthe strongest interaction exists in a short CuCu bond, the calculated results cannot be accepted easily. Consequently, we performed
inelastic neutron scattering (INS) measurements to determine experimentally the spin
system.2) INS measurements were carried out
on the thermal neutron triple-axis spectrometer TAS-2. The ﬁnal neutron energy was ﬁxed
at 13.7 meV. The collimation was guide-80’sample-80’-oepn.
The circles in the inset of Fig. 1 show
a constant-Q (scattering vector magnitude)scan spectrum. An asymmetric broad inelastic magnetic peak is observed. We measured
constant-ω (energy transfer) scan spectra at
5.1 K and at 5, 6, 7, and 8 meV and summed
the four spectra (circles in Fig. 1). A clear Q
dependence is visible. The line in Fig. 1 indicates the spherical average of the scatteringfunction of the alternating chain with the CuCu distance of 5.20 Å in the strongest interaction and is consistent with the experimental
result. In an alternating chain with strong
dimerization (J4  J1 ), the scattering intensity is strong at the bottom (spin gap) and
top of the dispersion. For that reason, we ﬁt原子炉：JRR-3

装置：TAS-2(T2-4)

ted a summation of two Gaussians (solid line)
to the experimental spectrum in the inset of
Fig. 1. The summation reproduces well theexperimental spectrum. Two peak energies
are about 6.2 and 8.0 meV (72 and 93 K). The
susceptibility of the AF alternating chain with
J4 = 80 K and J1 = 14 K (α ≡ J1 /J4 = 0.18)
agrees well with the experimental one.2) The
value 0.18 of α is almost the same as 0.17 in
the calculated results.1) The spin gap value in
the AF alternating chain is 72 K and is thesame as obtained in the INS measurements.
The higher energy 93 K is close to the energy
at the top of the dispersion in the AF alternating chain (J4 + 1/2J1 = 87 K). Consequently,
we could conclude that the spin system was
the AF alternating chain with J4 = 80 K and
J1 = 14 K and that the J4 bond with the long
Cu-Cu distance had the strongest exchangeinteraction.
 )$ (* 
)
' !(
& 
#$% 
"
! 
 
 

+

,

-/. 0 21.  43657 8 
  

9 0 >? @
:7  . <; =  57 8            Figure 1: Constant-ω and Q (inset) scan spectra.

References
1) H. B. Yahia et al. : Inorg. Chem. , 45, pp. 55015509 (2006).
2) M. Hase et al. : Phys. Rev. B , 76, pp. 134403
1-5 (2007).

分野：中性子散乱（磁性）㻙㻌 㻝㻡㻥㻌㻙

JAEA-Review 2011-050

1-2-56
Multi-step Magnetic Transition in Non-centrosymmetric Compound CeCoGe3
K. Kaneko1 , N. Metoki1 , T. D. Matsuda1 , A.Thamizhavel3 , T. Takeuchi2 ,Y. Haga1 ,R. Settai3 , Y. Ōnuki1,3
Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Naka, Ibaraki 319-1195
2
Low Temperature Center, Osaka University, Toyonaka 560-0043
3
Graduate School of Science, Osaka University, Toyonaka 560-0043

A discovery of the heavy fermion superconductivity in non-centrosymmetric compounds
CePt3 Si1) and CeT Si3 (T =Rh2) , Ir3) ) attracts a considerable interest, since exotic
superconducting properties are expected under the lack of inversion symmetry. Following the discovery of CeT Si3 , superconductivity was also found in isomorphous CeCoGe3
with Tsc =0.7 K under pressure of 5.5 GPa
5) . At ambient pressure, CeCoGe exhibits
3
multi-step magnetic transitions at TN1 =20 K,
TN2 =11.5 K and TN3 =7.5 K4) . The magnetic
structure of the ground state and the natureof the multi-step transitions have not beenclariﬁed so far. The present work aims toreveal the magnetic structure of the groundstate in CeCoGe3 by neutron diﬀraction.

q 2 measured at 2.9 K. Since no trace of magnetic peak was found in the (0 0 l) line, the directions of the magnetic moment corresponding to both q 1 and q 2 are parallel to thetetragonal c-axis. This direction of the magnetic moment is consistent with an anisotropy
in the magnetization measurement4) and is incontrast to CeT Si3 (T =Rh2) , Ir3) ). The coexistence of q 1 and q 2 suggests that the sizeof the ordered moment is not unique in the
ground state. The detailed magnetic structure analysis is now in progress.

A single crystalline sample of CeCoGe3 wasgrown by ﬂux method. Neutron diﬀraction
experiments were carried out on the two-axis
diﬀractometer MUSASI and thermal tripleaxis spectrometer TAS-2, both installed at
JRR-3. Neutrons with a wavelength of 2.44 Å
and 2.359 Åwere used in MUSASI and TAS-2,
respectively, with the PG ﬁlter in order to remove the higher order contamination. The
single crystal was mounted with the (h 0 l)
horizontal scattering plane.

counts / 150 s

1

Figure 1 shows the line scan proﬁle alongthe (1 0 l) in the reciprocal space of CeCoGe3
taken at 2.9 K. The superlattice reﬂection wasobserved at (1 0 1/2). The additional weak
peak at (1 0 1/4) was also found together with
its higher order harmonics of (1 0 3/4), indicated by arrows. At 25.0 K above TN1 , thesesuperlattice peaks were not observed. Therefore the propagation vectors of the groundstate are determined to be q 1 =(0 0 1/2) andq 2 =(0 0 3/4). The inset of Fig. 1 shows (0 0 l)
scan proﬁles at respective positions to q 1 and
原子炉：JRR-3

装置：TAS-2(T2-4)

150 (0 0 1/2)

300

100
countsCeCoGe3(1 0 l)
2.9 K

50
100

7.4 7.2(0 0 7/4)

7.0

200
50
25.8 25.6 25.4
( deg. )

100

0

0.2

0.4

0.6

0.8

1.0

( 1 0 l ) ( r. l. u. )Figure 1: The line scan proﬁle along the (1 0 l) of
CeCoGe3 taken at 2.9 K The inset shows the (0 0 l)
scan at l=1/2 and 7/4 measured at the same temperature.

References
1) E. Bauer et al., Phys. Rev. Lett. 92, 027003 (2004).
2) N. Kimura et al., Phys. Rev. Lett. 95, 247004(2005).
3) I. Sugitani et al., J. Phys. Soc. Jpn. 75, 043703(2006).
4) A. Thamizhavel et al., J. Phys. Soc. Jpn. 74, 1858
(2005).
5) R. Settai et al., Physica B 310, 844 (2007).

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JAEA-Review 2011-050

1-2-57
Pressure-Induced Magnetic Quantum Phase Transition in Coupled
Spin Dimer System KCuCl3
T. Ono, J. Kawakami, H. Tanaka, T. Osakabe1 and K. Kakurai1
Department of Physics, Tokyo Institute of Technology, Meguro-ku, Tokyo 152-8550
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

due to applied pressure is clearly observed.
The solid lines are the calculated results using
5

4

E (meV)

KCuCl3 is an interacting spin dimer system, which undergoes a pressure-induced
quantum phase transition (QPT) from agapped ground state to an antiferromagnetic
state at a critical pressure of Pc  8.2 kbar 1) .
An analysis of magnetic susceptibilities hasrevealed that the intradimer interaction decreases with pressure and the sum of interdimer interactions increases. This causes theshrinkage of the gap, which leads to the pressure induced QPT, as summarized in Fig. 1.
To clarify the pressure dependence of individual magnetic interactions in KCuCl3 , we investigated the magnetic excitations under hydrostatic pressures by neutron inelastic scattering experiments. This experiment is thecontinuation of the published study for thepressure at P = 4.7 kbar 2) .

3

2

KCuCl3
T = 1.4K

P = 0 kbar
P = 4.7 kbar
P = 6.4 kbar

10
0.5 0.4 0.3 0.2 0.1 0.0 0.1 0.2 0.3 0.4 0.5

Q = (0,0,1+2h)

Q = (h,0,0)

Figure 2: Dispersion relations in KCuCl3 measured at
4.7 and 6.4 kbar for Q along (0, 0, 1 + 2h) and (h, 0, 1).

RPA approximation 3) with eﬀective exchange
parameters listed in Table 1. The experiments
above the critical pressure is ongoing.
Table 1: Intradimer and eﬀective interdimer interactions in KCuCl3 in meV unit for P = 0, 4.7 and 6.4
kbar. The notational used here follows Ref. 3).

P [kbar]ambient
4.7
6.4

Figure 1: Pressure dependence of the gap Δ.

Neutron inelastic scattering experiments
was performed using LTAS spectrometer withthe collimation sequence guide-80’-80’-open
and with a ﬁxed ﬁnal neutron energy Ef =3.5 meV. The cylindrical high-pressure cellused was identical to that was used in Ref. 2).
Figure 2 shows the dispersion relations for
Q along (0, 0, 1 + 2h) and (h, 0, 1) measured
at P = 6.4 kbar together with the preceding
results. The softening of magnetic excitations
原子炉：JRR-3

装置：LTAS(C2-1)

J
4.34
3.65
3.29

J1eﬀ
-0.42
-0.62
-0.52

J2eﬀ
0.90
0.86
0.82

J3eﬀ
0.56
0.86
0.82

References
1) K. Goto, M. Fujisawa, H. Tanaka, Y. Uwatoko, A.
Oosawa, T. Osakabe, and K. kakurai: “J. Phys.
Soc. Jpn.”, 75 064703(2006).
2) K. Goto, T. Osakabe, K. Kakurai, Y. Uwatoko,
A. Oosawa, J. Kawakami, and H. Tanaka: “J.
Phys. Soc. Jpn.”, 76 053704(2007).
3) A. Oosawa, T. Kato, H. Tanaka, K. Kakurai, M.
Müller and H. -J. Mikeska: “Phys. Rev. B”65094426 (2002).

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JAEA-Review 2011-050

1-2-58Magnetic Structural Analysis of Magnetic Multilayers
by Complementary Use of X-ray and Neutrons
M. Takeda1,2,3 , D. Yamazaki1,2 , K. Soyama1,2 , R. Maruyama2 , M. Hino4 , T. Hirano5
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency (JAEA),
Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan
2
J-PARC Center, Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan3
New Industry Creation Hatchery Center, Tohoku Univ., Aramaki Aoba,
Aoba-ku, Sendai-shi, Miyagi, 980-8579, Japan
4
Kyoto University Reactor, Kyoto University, Kumatori-cho,Sennan-gun, Osaka, 590-0494,Japan
5
Hitachi Research Laboratory, Hitachi Ltd., Ohmika-machi, Hitachi-shi, Ibaraki, 319-1292, Japan

A read sensor head of a hard disk drive hasa layered structure and consists of several ferromagnetic (F), antiferromagnetic (AF), andnonmagnetic layers. Much attention is now
paid to the magnetic structure near the interfaces between the F and the AF layers in development of the high performance read sensors because a stable pinning of magnetization of F layer by AF layer is very sensitive
to the magnetic structure near the interfaces.
Complementary use of X-ray and neutron reﬂectometry is the most powerful and nondestructive tool to investigate such buried internal magnetic structures.
Figure 1 (a) shows the polarized neutron reﬂectivities from a multilayer which
is a part of a read sensor under a magnetic ﬁeld of 1.8 kOe using SUIREN.
The structure of the sample is described as
Si/Ta(5nm)/Ru(5nm)/MnIr(5nm)/CoFe(2nm)/Cu(1nm)/Ru(2nm). The length of the sample in the scattering plane was 35 mm, andthe height was 25 mm. The angle divergenceof the incident beam was controlled by two
sets of horizontal slits and was approximately
4 % (Δθ/θ) in the whole scan range.
The reﬂectivities with the spin-ﬂip clearly
indicate the existence of perpendicular component of internal magnetization under thisﬁeld. X-ray reﬂectivity of the same sample isalso displayed in Fig. 1 (b). This information
is not able to be obtained by the X-ray reﬂectivity measurements. On the other hand, thestatistics and the Q resolution of data in Fig.
1 (b) are better than those of polarized neutron reﬂectivities in Fig. 1 (a) even though
原子炉：JRR-3

装置：SUIREN(C2-2)

measuring time of the data in Fig. 1 (a) wasmuch longer than that of Fig. 1 (b). The layered internal structural information (paramagnetic one) is more accurately obtained fromthe X-ray reﬂectivity data. The complementary use of X-ray and neutron reﬂectometry
will give the reliable depth proﬁle of magnetization of this multilayer on the basis of thestructural information from the X-ray reﬂectivity measurements. Analyses of both data
are now in progress, and the results will bereported elsewhere.

Figure 1: Four kinds of polarized neutron reﬂectivities( a ), and X-ray one ( b ) from the same multilayer
which is a part of multilayer structure of a read sensor.

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JAEA-Review 2011-050

1-2-59Small-Angle Neutron Scattering Measurementsof Averaged Internal Structures in Nd-Fe-11 B Sintered Magnets
M. Takeda1,2,3 , J. Suzuki1,2 , D. Yamaguchi4 , T. Akiya 3 ,H. Kato3,5 , M. Sagawa3,6 , K. Koyama7
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency (JAEA),
Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan
2
J-PARC Center, Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan3
New Industry Creation Hatchery Center, Tohoku Univ., Sendai, Miyagi, 980-8579, Japan
4
Advanced Science Research Center, Japan Atomic Energy Agency (JAEA),
Tokai-mura, Naka-gun, Ibaraki, 319-1195, Japan
5
Department of Applied Mathematics and Physics, Yamagata Univ., Yonezawa,
Yamagata, 992-8510, Japan
6
Intermetallics Co., Ltd., Kyodaikatsura #303, 1-36 Goryo Ohara,
Nishikyo-Ku, Kyoto, 615-8245, Japan
7
Institute for Materials Research, Tohoku University, Sendai, Miyagi, 980-8577, Japan

We found that both of the integrated inten and q ⊥ M clearly corsities along the q//M
related with the coercivity values (Hc ): The
sample with the higher Hc has the higher
SANS intensity. Furthermore, imbalance of
the intensities between the spin-ﬂip (SF) andthe non-spin-ﬂip (NSF) components of the
SANS using the polarized neutrons along the direction was induced by the magnetic
q ⊥ M
 (Fig. 1), while SF
ﬁelds applied parallel to M
and NSF components were equal to each otherin zero external magnetic ﬁeld. The degreeof imbalance is diﬀerent among the samples
with the diﬀerent Hc . This suggests that the
原子炉：JRR-3

装置：SANS-J-II(C3-2)

magnetic inhomogeneity in the scale of 100 200 nm seems to aﬀect the Hc . Such inhomogeneity inside the grain has been thought tohave little eﬀect on Hc . Present work givesa hint to achieve the high-coercivity Dy-free
Nd-Fe-B sintered magnet.
(a) 0 Oe/On-Off

120(b) 10 kOe/On-Off

120

100

400

100

300

80

200
60
100
40

0
-100

20

0

Y (ch)Y (ch)

Neodymium iron boron (Nd-Fe-B) sinteredmagnets are now widely used because of thehighest (BH)max among the commerciallyavailable permanent magnets. At the present,
Dy, which is one of the rare metals, has tobe added to keep the coercivity especially inthe operational temperatures higher than theroom temperature. The key to achieve thehigh-cercivity Dy-free Nd-Fe-B sintered magnets is how to control the grain size and thestructure near the grain boundary. We have
performed the small-angle neutron scattering(SANS) measurements of the Nd-Fe-11 B sintered magnets using unpolarized and polarized neutrons to obtain the averaged internal
structures of samples with the diﬀerent coercivity introduced by applying high magnetic
ﬁelds during the annealing1) .

400
300

80

200
60
100
40

0
-100

20

0
0

20

40

60

80

100

120

0

X (ch)

20

40

60

80

100

120

X (ch)

Figure 1: Diﬀerences of the intensity between SF and direction on the
NSF components along the q ⊥ M
2D-PSD: (a) the map in zero magnetic ﬁeld and (b).
in the ﬁeld of 10 kOe applied parallel to M

This work was partially supported by
the Ministry of Economy, Trade and Industry (METI), and New Energy and Industrial Technology Development Organization(NEDO), Grant-in-Aid for ”Development oftechnology for reducing dysprosium usage ina rare-earth magnet” in ”Rare Metal Substitute Materials Development Project”.
References
1) H. Kato, T. Miyazaki, M. Sagawa, and K. Koyama,Appl. Phys. Lett., 84 (2004) 4230. (2007) s474.

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JAEA-Review 2011-050
















1.  ਛᕈሶᢔੂ 3 ᒝ⋧㑐㔚ሶ♽

1. Neutron Scattering

3 Strongly Correlated Electron
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JAEA-Review 2011-050

1-3-1

Magnetic excitations in halogen-bridged nickel complex
S. Itoh and K. Nakajima*High Energy Accelerator Research Organization, Tsukuba, 305-0801, *Japan Atomic Energy
Agency, Tokai, 319-1195
Halogen-bridged metal complexes witha one-dimensional (1D) mixed-valence X-M(II)-X-M(IV)-X- structure have beenstudied as a Peierls distorted chain system with a strong electron-lattice interaction resulting from the off-centeredposition of halogen between neighboring metal atoms. Among these compounds, [NiBr(chxn)2]Br2 (chxn:1R, 2Rcyclohexanediamine) have a non-distorted
1D structure expressed as -Br-Ni(III)-BrNi(III)-Br-[1,2]. This spin structure implies
antiferromagnetic Heisenberg chains with
S = 1/2. Magnetic susceptibility measurements up to the room temperature suggested a large exchange constant of J ˜ 0.3
eV [2]. Optical studies have been revealed
that this system exhibits a 1D charge transfer insulator [3]. The observed optical properties can be explained by a 1D extended
Hubbard model [4], and it suggested J ˜ 0.4
eV, which is consistent with the result on
the susceptibility.
In order to detect magnetic excitations,
we previously performed an inelastic neutron scattering experiment on HER (C1-1)
at JRR3M in JAERI (Tokai) in 2002, by using 20 g of a single-crystal sample. However, we could not detect meaningful magnetic signals at the magnetic zone center atenergy transfers up to 1.5 meV at 1.4 K.
Recently, this system has been suggested
to be a spin-Peierls system with Tsp˜40Kfrom magnetic susceptibility study as wellas 81Br NQR study [5]. By applying the
BCS theory to the spin-Peierls system, thegap energy can be estimated to be approximately 6 meV from Tsp. At present, in order to investigate the spin-Peierls nature inthis system, an experiment was performedon PONTA (5G) at JRR3M in JAEA (Tokai),by using the same sample. Since, from theprevious experiment in 2005, we thoughtthat we could detect tiny magnetic signals
at low energy region at the magnetic zone,
we again tried to measure inelastic signals
to improve statistics at present. The experiment was performed at 8 K and 100 K (below and above TSP), however, we could
not detect meaningful magnetic signals because of huge incoherent inelastic signals
from hydrogen atoms. In order to detectmagnetic signals, deuteration of the sample
is essential. For the next time, we try to observe magnetic signals using a deuterated
sample.
References[1] K. Toriumi et al., J. Am. Chem. Soc. 111(1989) 2341.
[2] H. Okamoto et al., Phys. Rev. B 42 (1990)
10381.
[3] H. Okamoto et al., Phys. Rev. B 54 (1996)
8438.
[4] N. Tomita and K. Nasu, Phys. Rev. B 56
(1997) 3779.
[5] S. Takaishi et al., J. Am. Chem. Soc. 126(2004) 1614.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 99

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JAEA-Review 2011-050

1-3-2

Charge and magnetic order in 2d cobaltate Pr2-xCaxCoO4
H. Yoshizawa and K. Masuda
Neutron Science Laboratory, ISSP, The University of Tokyo
We studied the charge and spin order inthe 2d cobaltate Pr2-xCaxCoO4 in JFY2005
and 2006. For 0.39 < x < 0.5 where the holeconcentration is less than but close to x =0.5, the spin and charge order in the cobaltates has the checkerboard-type as shownin Fig. 1 (a). On the other hand, for x >0.5 where the hole concentration is larger
than half the number of the Co sites, incommensurate (IC) peaks appear with two
characteristic wave vectors, (δ, 0, 1) and(2 δ, 0, 1), with δ = 1-x. From their Qdependences, we identiﬁed the IC peaks
with (δ, 0, 1) to be magnetic and those with
(2 δ, 0, 1) to be structural. This indicatesthat the charge and spins form stripes asshown in Fig. 1 (b). This stripe order is similar to those observed in the underdoped region of cuprates and nickelates. It is however to note that in the overdoped (x > 0.5)
cobaltates the magnetic Co2+ ions form thedomain boundaries that separate the nonmagnetic Co3+ ions.
In order to understand an origin of this unusual spin-charge order, we studied its spin
dynamics in the JFY2007, and found thatits spin dynamics is governed by a strong
planar anisotropy and spin state transiton
from an intermediate to low spin state. The
detailed quantitative analysis is now underway.

Fig. 1. Schematic models for the checkerboard-typespin-charge order (left) and spin string order (right)
in PCCO.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 262

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JAEA-Review 2011-050

1-3-3
Variation of magnetic modulation for the antiferromagnetic states in
CeRh1−x Cox In5 ( x = 0, 0.5 and ∼ 0.7)
N. Oyama1 , M. Yokoyama1 , S. Oinuma2 , I. Kawasaki2 , H. Amitsuka2 , K. Tenya3 , T. J.
Sato4 , M. Matsuura4 and K. Hirota4
1 Ibaraki University, 2 Hokkaido University, 3 Shinshu University, 4 ISSP, The University ofTokyo
For a decade, there has been a growing interest in physical property near thequantum critical point (QCP) in the heavyfermion systems. The heavy-fermion compound CeRhIn5 orders in an incommensurate antiferromagnetic (AF) phase witha modulation of qh = (1/2, 1/2, 0.297)[1]. It is revealed in the Co-doped alloys
CeRh1− x Cox In5 [2] that the AF phase issuppressed with increasing x, and then disappears at xc ∼ 0.7. At the same time,superconductivity (SC) appears between
x = 0.4 and x = 1. Furthermore, recent
elastic neutron scattering experiments for
CeRh1− x Cox In5 with intermediate Co concentrations [3, 4] revealed that a commensurate magnetic order with a wave vector
qc = (1/2, 1/2, 1/2) develops at low temperatures. To elucidate the nature of these
AF phases, we have performed the neutron
scattering experiments for CeRh1− x Cox In5( x = 0, = 0.5, ∼ 0.7).
Single crystals of CeRh1− x Cox In5 weregrown by the In-ﬂux method. The samples were shaped into bar (typical size: ∼3 mm2 × 10 mm) in order to minimize theeffects of the neutron absorption caused by
Rh and In. Elastic neutron scattering experiments were carried out using triple-axis
spectrometers GPTAS and PONTA at the
JRR-3M research reactor of JAEA. Measurements were performed in the (hhl) scattering plane.
Figure 1 shows the neutron scattering
pattern obtained from the (1/2, 1/2, 1 + ξ)
(0 ≤ ξ ≤ 1) scan at 1.6 K. The incommensurate magnetic Bragg peaks were observed for x = 0, whose wave vector corresponds to qh ∼ (1/2, 1/2, 0.297). For
x = 0.5, we observed of the commensurate

magnetic Bragg peak with the modulationof qc = (1/2, 1/2, 1/2). In addition, forx ∼ 0.7, we have found that the qh peak position moves toward q1 ∼ (1/2, 1/2, 0.42),
together with the apperance of the qc peak.
From these results, we suggest thatthe commensurate magnetic correlation istightly coupled with SC.
References[1] W. Bao et al., Phys. Rev. B 62 (2000) R14621;
Phys. Rev. B 67 (2003) 099903(E).
[2] V.S. Zapf et al., Phys. Rev. B 65 (2001)
014508.
[3] M. Yokoyama et al., J. Phys. Soc. Jpn. 75(2006) 103703.
[4] S. Ohira-Kawamura et al., Phys. Rev. B 76
(2007) 132507.

Fig. 1. Antiferromagnetic Bragg-peak proﬁles at 1.6
K for CeRh1− x Cox In5 .

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 276

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JAEA-Review 2011-050

1-3-4
Evolution of Ferromagnetic and antiferromagnetic orders in Mn-doped CaRuO3
M. Yokoyama, H. Hagiya, N. Oyama, Y. Nishihara and H. Kawanaka1
Ibaraki University, 1 National Institute of Advanced Industrial Science and Technology
Temperature variations of these Braggpeak intensities [Fig. 2(b)] are consistent
with characteristics seen in the magnetization: the magnitude of magnetization ismarkedly suppressed below ∼ 90 K.
References[1] I. Felner et al.: Phys. Rev. B 66 (2002) 054418.
[2] V. Hardy et al.: Phys. Rev. B 73 (2006)
094418.
[3] V. Durairaj et al.: Phys. Rev. B 73 (2006)
214414.
[4] A. Maignan et al.: Phys. Rev. B 73 (2006)
024410.
[5] A.I. Shames et al.: Phys. Rev. B 70 (2004)
134433.

20

25

200

2

020

CaRu Mn O
0.6

0.4

3

200

30
35
2θ (deg)

121

15 K
290 K
111

101

110
011

Intensity(a)M (arb. units)

The relationship between metalinsulator transition and magnetism in
the transition-metal oxides is one of
the intriguing issues in the condensedmatter physics. The distorted perovskite
compound CaRuO3 (the GdFeO3 -type
orthorhombic structure; space groupPnma) is considered to be a paramagnetic metal located in the vicinity of themetal-insulator transition. It is revealed
that the ionic substitutions for the Rusite dramatically enhance the magnetic
correlation [1, 2, 3, 4]. We recently foundthat the substitution of Mn for Ru induces
both ferromagnetic and antiferromagnetic(AF) components in the magnetization,accompanying the variation of the electrical resistivity from metallic to insulating
behavior. These features are expected to
be attributed to the change of the d electronic state. To investigate the microscopic
properties of the d electrons in the intermediate Mn concentration range, we have
performed powder neutron diffraction
experiments for CaRu1− x Mnx O3 .
The
polycrystalline
samplesof
CaRu1− x Mnx O3 with x = 0.4 wereprepared by the solid-state method. The
neutron diffraction measurements for
powdered samples were performed in thetemperature range between 15 K and 290
K, using the HERMES spectrometer (IMR,
Tohoku Univ.) installed at the guide hall of
the research reactor JRR-3M of JAEA. The
wavelength of the incident neutron was
selected to be 1.8264 Å. Figure 1(a) shows
low-angle part of the neutron powder
diffraction proﬁles at 15 K and 290 K
for x = 0.4. The (110) and (011) Bragg
peaks are clearly observed at 15 K, which
attributes the occurence of the G-type
AF order. In addition, the enhancementof the (020) Bragg-peak intensity due toferromagnetic order was also detected.

40

45

(b)

150

G-AF
Ferro

100
50
0
0

50

100

150
T (K)

200

250

300

Fig. 1. (a) Neutron powder diffraction proﬁles at 15
K and 290 K, and (b) Temperature variations of thesquare of the ferromagnetic and antiferromagnetic
moment for CaRu1− x Mnx O3 with x = 0.4.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 283

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JAEA-Review 2011-050

1-3-5
Modulated-structure analysis of the high-valence aperiodic chain compounds,
Sr2k(Co1-xNix)O3 (k˜0.635, 0<=x<=1)
Masaaki ISOBE (A), Hideaki KITAZAWA (B), Kenji OHOYAMA (C)(A) Advanced Nano Materials Laboratory, National Institute for Materials Science; (B)Quantum Beam Center, National Institute for Materials Science; (C) Institute for Materials
Research, Tohoku University
The A2kMO3 (A: alkali-earth elements,
M: transition metals)-type compounds belong to a hexagonal class in Bravais lattices. This system has two types of onedimensional chain sub-lattices of [MO3]blocks and A ions, running along the caxis in the crystal structure. The atomic positions are incommensurately modulated
due to irrational-ratio periodicity of the
sub-lattices (c1/c2=k). Recently, we foundfrom static-magnetic measurements thatsolid-solution phases Sr2k(Co1-xNix)O3(k˜0.635, 0<=x<=1) can possess an unusual
high-valence (˜3.5+) state of the Co and Ni
ions throughout the x compositions. The
purpose of this experimental subject is tomake clear the true valence of the ions in
the Sr2k(Co1-xNix)O3 system, by precisely
analyzing the modulated crystal structure,including oxygen positions.
Neutron diffraction data for thepolycrystalline samples with compositions of Sr14Co11O33, Sr14Co8Ni3O33,
Sr9Co3.5Ni3.5O21 and Sr9Co2Ni5O21
were collected using the HERMES diffractometer (IMR, Tohoku Univ.) at room
temperature in a 2theta range from 7
to 157.95 degrees, in a step size of 0.05
degree. Incident thermal neutron beams
were monochromatized to a wavelengthof 1.8265 A with the 331 reﬂection ofa bent-crystalline Ge monochromator.
The modulated crystal structures ofSr2k(Co1-xNix)O3 were analyzed by
the Rietveld method using a computer
software, PREMOS91 [1], on the basis of
a superspace-group approach. The initial structure model was constructed bymaking reference to the structure model
proposed by Onoda et al. for Sr1.145TiS3[2]. The super-space groups, P-R3m/1s

and R-P31c/111, were adopted for theﬁrst- ((Co,Ni)O3) and the second- (Sr)subsystems, respectively.
Figures 1 (a) and (b) show crystal structures illustrated using the reﬁned
structure parameters for the sample ofSr14/11(Co8/11Ni3/11)O3 (Rwp=5.44%).
The (a) is a projection along the c-axis, andthe (b) is a projection perpendicular to thec-axis of one of the [(Co,Ni)O3] chains andthe neighboring Sr atoms. The lattice parameters are a=9.4761(2) A, c1=2.54105(8)A, and k(=c1/c2)=0.63505(5). The ﬁgure (b)reveals sequence of the polyhedron types,
i.e. a trigonal prism (TP) and an octahedron(Oh), around the Co and Ni atoms.
Figure 1 (c) shows Co,Ni-O distances
as a function of the internal forth coordinate t’ for the (3+1)-dimensional
incommensurate structure model of
Sr14/11(Co8/11Ni3/11)O3. The O(+z) andthe O(-z) curves indicate oxygen atoms
above and below the Co/Ni atom along thec-axis, respectively. The shaded area corresponds to the TP sites, and the non-shaded
area to the Oh sites. The [(Co,Ni)O3] chain
comprises 27% TP and 73% Oh sites. The
ﬁgure (c) indicates that in most of the TP
sites, both the Co,Ni-O lengths, O(+z) andO(-z), are simultaneously lengthened ascompared to those in the Oh sites. We also
analyzed occupancy probabilities of the Co
and Ni atoms at the M site, as a functionof t’. It was found that the Ni atoms prefer
the TP sites to the Oh sites, and that the
Co atoms are selectively situated at the Oh
sites. The bond valences were calculated
from the Co,Ni-O distances and the occupancy probabilities. The values are ˜2.3+
for the TP sites and ˜3.4+ for the Oh sites on
average. It suggests that the high-valence

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state can appear exclusively at the Oh sites.
References[1] A. Yamamoto, Acta Crystallogr. A49(1993) 831; ibid. A52 (1996) 509.
[2] M. Onoda, M. Saeki, A. Yamamoto, and
K. Kato, Acta Crystallogr. B49 (1993) 929.

Fig. 1.
(a, b) Crystal structure of
Sr14/11(Co8/11Ni3/11)O3; (c) Co,Ni-O distances as a function of the internal forth coordinate
t’.

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1-3-6

Magnetic phase diagram under low temperature and high pressure in RVO3
D. Bizen(A), H. Nakao(A), K. Iwasa(A), Y. Murakami(A), T. Osakabe(B), S.
Miyasaka(C), Y. Tokura (D,E)(A) Tohoku Univ., (B) JAEA, (C) Osaka Univ., (D) The Univ. of Tokyo, (E) CERC
the spin state when the orbital ordering of
the ground state is changed by applying
pressure. The result indicates a strong coupling between the spin state and the orbital
state in RVO3 system.
[1] S. Miyasaka et al., Phys. Rev. B 68 (2003)
100406.
[2] D. Bizen et al., J. Magn. Magn. Mater.
310 (2007) 785.
7

4.3GPa2.4GPa
1.0GPa0GPa

6Intensity (arb. units)

RVO3 (R: rear earth or Y) shows various physical properties coupled with thespin and orbital states. [1] The orbital stateis strongly coupled with the lattice distortion, i.e. Jahn-Teller distortion. Hence thepressure effect for the orbital state interests
us, and the pressure-temperature phase diagram of the V 3d-orbital state was investigated by x-ray diffraction under highpressure and low-temperature. [2] It elucidated that the C-type orbital ordering (COO) is stabilized as compared with the Gtype orbital ordering (G-OO) by applyinghydrostatic pressure. The spin state coupled with the orbital state is also an important problem for this system. Therefore, thespin state in TbVO3, of which the groundstate of 3d-orbital changes from the G-OO
to the C-OO by applying pressure, was investigated under high-pressure and lowtemperature using a hybrid anvil cell.
In order to determine the magnetic ordering, the magnetic scattering was measured by using the triple-axis spectrometer TOPAN. The temperature dependenceof the magnetic peak intensities was measured at several pressures as shown in theﬁgure. At ambient pressure (0 GPa), themagnetic peak at (0 1 0) reﬂecting the Ctype spin ordering (C-SO) was observed
below the magnetic transition temperature.
With increasing pressure, the C-SO phaseis suppressed and ﬁnally disappears. On
the other hand, the magnetic peak at (0 1
1) reﬂecting the G-type spin ordering (GSO) appears above 1.0 GPa, and the magnetic transition temperature remarkably increases with applying pressure. As compared with the orbital phase diagram [2],it becomes clear that the G-SO phase corresponds to the C-OO phase and the C-SO
phase appears in the G-OO phase. Namely,
we could clearly determine the changing

5(0 1 0)4
3
2(0 1 1)

1
0
0

50

100

150

200

250

Temperature (K)Fig. 1. Temperature dependence of the magnetic
peak intensities at (0 1 1) and (0 1 0), which correspond to G-OO and C-SO, respectively.

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1-3-7

Study on thermoelectric properties and misﬁt-structures in Y doped Ca3Co4O9
H.Nakatsugawa, H.M.Jeong, and K.Nagasawa
Yokohama National University 79-5 Tokiwadai Hodogaya Yokohama 240-8501 Japan
Since the discovery of large thermoelectric power in the layered compounds
NaCo2O4 and Ca3Co4O9, misﬁt-layered
cobalt oxides particularly have attracted
much interest as candidates for thermoelectric (TE) materials. The polycrystalline
Ca3Co4O9 sample typically exhibits S=130
μ V/K, ρ=15m Ω cm and κ=1.0W/mK at
room temperature. For practical use, an appreciable decrease in ρ must be achieved
because ρ=15m Ω cm at room temperature is about one order of magnitude
higher than that of Bi2Te3-based TE materials. In this study, we have employeda high-resolution powder neutron diffraction technique to investigate the weakmodulated crystal structure of trivalent Y
ion doped Ca3Co4O9 polycrystalline samples. This study was carried out to investigate the valence state of Co ions both in the
CoO2 sheet and in the RS-type BL subsystems.
The polycrystalline samples of [(Ca1xYx)2CoO3]0.62CoO2 (0 ≦ x ≦ 0.04) wereprepared by the conventional solid-state reaction method. The sample homogeneityand crystallinity were conﬁrmed by meansof the powder Neutron diffraction (ND)
technique. Tne ND data were collected at
293K using the Kinken powder diffractometer for high efﬁciency and high resolution measurements (HERMES) of Institute for Materials Research (IMR), Tohoku
University, installed at the JRR-3M reactor in Japan Atomic Energy Research Institute (JAERI), Tokai. The incident neutron
beam was monochromatized at λ=1.8265Å. The ND data were analyzed using a
Rietveld reﬁnement program PREMOS 91
designed for modulated structure analyses. The crystal structures and interatomic
distance plots were obtained with the useof PRJMS and MODPLR routines, respectively, both were implemented in the PRE-MOS 91 package.
First, we assumed the superspace group of
C2/m(0 p 0)s0 for the crystal structure of[(Ca0.98Y0.02)2CoO3]0.62CoO2 (x = 0.02),
and assigned the CoO2 sheet for subsystem 1 and the RS-type BL for subsystem2.
In this superspace group, the CoO2 sheet
has C2/m symmetry while the RS-type BL
subsystem has C21/m symmetry.
After two or three reﬁnement cycles,
the modulation of the atomic positions in
x=0.02 was introduced, considering up to
the second order of cosine and sine components of the Fourier terms, i.e., Ai (i =0, 1, 2) and Bi (i = 1, 2). Figure 1 shows
the observed, calculated and difference intensities of the HERMES data for x = 0.02.
Short vertical lines below the patterns indicate the peak positions of the main (upper) and satellite (lower) reﬂections for the
CoO2 sheet and RS-type BL subsystems.
The difference between the observed andcalculated patterns is shown below the vertical lines. The ﬁnal Rwp factor is 5.91 %and the lattice parameters are reﬁned to a
= 4.8300(5) Å, b1 = 2.8220(1) Å for CoO2
sheet, b2 = 4.5517(1) Å for RS-type BL subsystem, c = 10.838(9) Å and β= 98.13(8) °.

Fig. 1. Observed, calculated and difference intensities of ND data for [(Ca0.98Y0.02)2CoO3]0.62CoO2(x=0.02).

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1-3-8
Magnetic excitation in a non-centrosymmetric pressure-induced superconductor
CeRhSi3
N. Aso, H. Miyano, H. Yoshizawa, N. KimuraA , T. KomatsubaraA , H. AokiA
NSL-ISSP Univ. of Tokyo, Graduate School Sci. Tohoku Univ.A
ﬁxed energy of kf = 1.55 Å−1 using the horizontally focused analyzer. One can recognize an energy-broad magnetic signal at theenergy loss side, which is almost wave vector independent. Thus we did not observe
any signal corresponding to the LSDW ordering wave vector. We will plan to go to
the lower energy in the next.
References[1] N. Kimura et al., Phys. Rev. Lett. 95, 247004(2005).
[2] Y. Muro et al., J. Phys. Soc, Jpn. 67, 3601
(1998).
[3] A. Krimmel et al., Appl. Phys. A 74 Suppl.,
S695 (2002).
[4] N. Kimura et al., Physica B 294-295, 280(2001).
[5] N. Aso et al., J. Magn. Magn. Mater. 310(2007) 302.

Intensity / M1420k (~7-16min)Coexistence between magnetism and superconductivity (SC) is the central issue incondensed matter physics. Recently noncentrosymmetric heavy-fermion superconductor CePt3 Si and UIr were reported.
From the fundamental point of view ofsymmetry, the discovery of these materials
are very surprising because there are twobasic symmetries which are considered indispensable to form Cooper pair: time reversal symmetry and parity. The former isimportant for Cooper pairing in any casewhile the latter is mandatory for pairingin the triplet channel. Thus there is a lotof discussions for the non-centrosymmetric
SC at present.
Kimura et al. [1] discovered another noncentrosymmetric superconductor CeRhSi3
with the crystal structure of BaNiSn3 -type(I4mm). [2] CeRhSi3 exhibits the antiferromagnetic (AFM) ordering below TN = 1.6 K
at ambient pressure (P). By increasing theP, TN shows a maximum around 0.7 GPa,then gradually decreases. SC appears ina wide P range from 1.2 to 2.3 GPa (andmore). Concerning the magnetic structure, there was only one neutron diffraction
work on polycrystalline samples, [3] which
exhibits no magnetic reﬂections with possible maximum magnetic moment of 0.25
μB /Ce. In the last year we have ﬁrst determined the magnetic structure using thesingle crystalline CeRhSi3 , [5] indicating
the longitudinal spin density wave (LSDW)with the wave vector of k = (0.215, 0, 0.5)
and the Ce staggered moment of ∼ 0.1
μB /Ce.
This year we tried to examine the lowenergy magnetic excitations below TN = 1.6
K. Figure 1 shows the inelastic scattering
proﬁle at Q = (0.215, 0, 1.5) and T = 0.76 K
obtained at the HER spectrometer with the

CeRhSi3, #20725
Q=(0.215,0,1.5)
T=0.76K
80

100

60
40
20
0
-2

-1

0

1

2

3

Energy (meV)Fig. 1. Inelastic neutron scattering proﬁle at Q =(0.215, 0, 0.5).

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1-3-9

Neutron diﬀraction under pressure in CeRhIn5
N. Aso, K. Ishii, H. Yoshizawa, T. FujiwaraA , Y. UwatokoB , G. F. ChenC , N. K. SatoC
NSL-ISSP, Univ. of Tokyo, Graduate School of Sci. and Engineering, Yamaguchi Univ.A ,ISSP, Univ. of TokyoB , Graduate School of Sci., Nagoya Univ.C
4.9 K (above TN ). Here we would like toemphasize that our results surpassed thepast ones [4, 5] for the intensity of about 70
counts/min and SN ratio of ∼ 1.3. These
arise from the optimization of both the
crystal and pressure cell sizes.
The incommensurability δ in the propagation vector τ = (0.5, 0.5, δ) smoothly increase from 0.297 at P = 0 to 0.326 at 1.22
GPa, which is qualitatively different fromthe previous results. [4, 5] We believe thatthese difference comes from the used pressure transmitting media.
References[1] H. Heeger et al., Phys. Rev. Lett. 84, 2986
(2000).
[2] T. Park et al., Nature 440, 65 (2006).
[3] G. F. Chen et al., Phys. Rev. Lett. 97, 17005(2006).
[4] S. Majumdar et al., Phys. Rev. B 66, 212502(2002).
[5] A. Llobet et al., Phys. Rev. B 69, 024403(2004).
800

Intensty (counts/5min)

The interplay between magnetism andsuperconductivity (SC) is the interestingand important issue on condensed matterphysics. In CeRhIn5 [1, 2], it was very difﬁcult to establish the coexistence of both twophases under pressure (P) because of theinhomogeneity of the P. There was open
to argument if the coexistence is intrinsic.
Very recently G.G. Chen et al. [3] reported that high-quality single crystalline
CeRhIn5 display the SC at TSC ∼ 90 mKeven under ambient P and its P-T phase diagram is drastically renewed. These ﬁndings indubitably indicate that the identicalf electron plays both roles of SC and AFM.
Therefore CeRhIn5 is a very important material for the investigations on the coexistence of SC and AFM. To elucidate the coexistence mechanism of both SC and AFM,
it is very useful to perform neutron diffraction under P which is a very powerful tool
to directly determine the magnetic structure of the system.
The main goal of our study is to observe any changes through the SC transition temperature TSC in CeRhIn5 . On theother hand, since the strong neutron absorption of Rh, In nuclei and pressure cell
itself make the magnetic neutron diffraction under P extremely difﬁcult, there has
been little good information on the magnetic structure under P [4, 5].
In this work, we prepared a small CuBebased pressure cell and succeeded in detecting magnetic reﬂections under P up
to 1.5 GPa at the ISSP/GPTAS and HQR
spectrometers in the research reactor JRR3/JAEA. Figure 1 shows neutron diffraction proﬁle thorough Q = (0.5, 0.5, L) at P ∼0.25 GPa. One can clearly recognized a pairof magnetic peaks at L ∼ 1.298 and 1.702
at T = 0.75 K (below TN ), which are trulyof magnetic origin since they disappear at

CeRhIn5, P~0.25GPa

700
600
500
400
300

JRR-3/GPTAS, ki=3.83Å
200
1.2

1.3

1.4

0.75K
4.9K

-1

1.5

1.6

1.7

1.8

(0.5,0.5,L)

Fig. 1. Incommensurate magnetic Bragg reﬂectionsat P ∼ 0.25 GPa.

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1-3-10Two-dimensional magnetic excitations in CeRhIn5
N. Aso, H. Miyano, H. Yoshizawa, G. F. ChenA , N. K. SatoA
NSL-ISSP, Univ. of Tokyo, Graduate School of Sci., Nagoya Univ. A
This year we have been continuing tostudy the DS in CeRhIn5 at the ISSP/HER
spectrometer in the research reactor JRR3/JAEA. Figure 1 shows inelastic neutron
scattering spectrum at constant energy ofh̄ω = 0.8 meV in the (h, h, l)-zone at and T =1.4 K. One can clearly recognize a strong intensity along the (0.5, 0.5, l) line, indicatingthat the low-energy magnetic excitation is a
two-dimensional nature. We are now continuing to study the overview of the lowenergy part of its DS in CeRhIn5 .
References[1] H. Heeger et al., Phys. Rev. Lett. 84 (2000)
4986; S. Kawasaki et al., Phys. Rev. B 65
(2002) 20504; T. Muramatsu et al., J. Phys.
Soc. Jpn. 70 (2001) 3362.
[2] T. Park et al., Nature 440 (2006) 65.
[3] G. F. Chen et al., Phys. Rev. Lett. 97 (2006)
17005.
[4] N. Aso et al., NSL-ISSP Activity Report 14(2007) 227.
T=1.4K
Intensity / M1420k (~10min)

The interplay between magnetism andsuperconductivity (SC) is the interestingand important issue on condensed matterphysics. Although it has been considered
to be exclusive over quantum critical point(QCP), it is now widely accepted that bothSC and antiferromagnetism (AFM) coexist in the vicinity of QCP in the systemsof the pressure (P)-induced superconductor CePd2 Si2 , CeIn3 , and CeRhIn5 [1, 2] andso on after a lot of energetic investigations.
Since it, however, was very difﬁcult to establish the coexistence of both two phases
under P because of the inhomogeneity of
the P, there was open to argument if thecoexistence is intrinsic. Very recently G.G.
Chen et al. [3] reported that high-quality
single crystalline CeRhIn5 display the SC
at TSC ∼ 90 mK even under ambient P
and its P-temperature (T) phase diagram isdrastically renewed. These ﬁndings indubitably indicate that the identical f electron
plays both roles of SC and AFM. Therefore CeRhIn5 is a very important material
for the investigations on the coexistence ofSC and AFM. To elucidate the coexistencemechanism of both SC and AFM, it is very
useful to perform inelastic neutron scattering which is a very powerful tool to directly
observe the dynamical spin susceptibility(DS) of the system. The main goal of ourstudy is to determine the wave vector dependence and its energy scale of the DS in
CeRhIn5 , and to ﬁnd out the connection between SC and the DS.
On the other hand, since the Rh and In
nuclei are strong neutron absorbers, there
has been little information on low-energy
magnetic excitations by inelastic neutron
scattering studies. In the last year, we succeeded in detecting the low energy magnetic excitations at the AFM ordering wave
vector Q = (0.5, 0.5, 2.7) by using a lot oflarge single crystals of CeRhIn5 . [4]

150
150

100

100

50

50

0
1

0.8
0.6

L

0.4

in (H,H,L)

0.2
0

0.2

0.4

0.6

0

H

in (H,H,L)

Fig. 1. Inelastic neutron scattering proﬁles in the(h, h, l)-zone at h̄ω = 0.8 meV and T = 1.4 K.

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1-3-11
Search for magnetic excitation in a heavy fermion superconductor CeCoIn5
N. Aso, H. Miyano, H. Yoshizawa, T. FujiwaraA , G. F. ChenB , N. K. SatoB
ISSP, Univ. of Tokyo, Graduate School of Sci. and Engineering, Yamaguchi Univ.A ,Graduate School of Sci., Nagoya Univ.B
The interplay between magnetism andsuperconductivity (SC) is the interestingand important issue on condensed matterphysics. A recently discovered series of
CeMIn5 (M = Rh, Co and Ir) has the highest SC transition temperature Tc = 2.3 K forheavy fermion materials. [1] It is believedthat such a high Tc can be realized by strong
antiferromagnetic (AFM) ﬂuctuations. For
example, CeRhIn5 exhibits an incommensurate AFM ordering with the wave vectorof τ= (0.5, 0.5, 0.297). [2] Very recently G.G.
Chen et al. [3] reported that high-quality
single crystalline CeRhIn5 display the SC
at Tc ∼ 90 mK even under ambient pressure (P) and its P-T phase diagram is also
drastically renewed. These ﬁndings indubitably indicate that the identical f electron
plays both roles of SC and AFM. Therefore
CeRhIn5 is a very importance material forthe investigations on the coexistence of SC
and AFM. To elucidate the nature of bothSC and AFM, it is very useful to performinelastic neutron scattering which is a very
powerful tool to directly observe the dynamical spin susceptibility of the system.
In this context, we ﬁrst succeed in observing the low-energy magnetic excitations in CeRhIn5 . [4] Inelastic neutron scattering spectrum at constant energy of h̄ω= 0.8 meV in the (h, h, l)-zone and T = 1.4
K clearly showed a strong intensity alongthe (0.5, 0.5, l) line, indicating that thelow-energy magnetic excitation is a twodimensional nature. Thus the main goal of
our study is to detect the low-energy magnetic excitations in CeCoIn5 and to determine its energy scale of the dynamical susceptibility CeCoIn5 , and to compare thembetween CeRhIn5 and CeCoIn5 .
Single crystals of CeCoIn5 were grownby In-ﬂux method. Inelastic neutron scattering experiments were carried out at 4G(GPTAS) and C1-1 (HER) spectrometers in
the research reactor JRR-3. (hhl)-zone wasselected as the scattering plane. The crystals with the total mass of ∼ 0.5 gram werealigned with the total area of ∼ 300 mm2
and were cooled down to T = 1.5 K.
We observed very weak low-energy excitations below 1.5 meV at Q = (0.5, 0.5,2.3), (0.5, 0.5, 2.5) and (0.5, 0.5, 2.7). Unfortunately we can not identify whether
these intensities are Q-dependent nor identify that this signal is of magnetic origin.
The possible reasons are that the used crystals are not enough for the inelastic neutron
scattering study and that the temperatureof 1.5 K is not low enough for Tc = 2.3 K.
Note: After our work, we noticed thatthe group of Collin Broholm detected thelow-energy magnetic excitations aroundthe commensurate AFM wave vector τ =(0.5, 0.5, 0.5) in CeCoIn5 with total mass of∼ 5 gram. A sharp spin resonance (h̄Γ <0.07 meV) at h̄ω = 0.60 ± 0.03 meV develops in the SC state and disappears above
Tc . [5]References[1] C. Petrovic et al., J. Phys.: Condens. Matter
13, L337 (2001).
[2] W. Bao et al., Phys. Rev. B 62, R14621(2000); ibid 63, 219901(E) (2001); ibid 67,
099903(E) (2003).
[3] G. F. Chen et al., Phys. Rev. Lett. 97 (2006)
17005.
[4] N. Aso et al., NSL-ISSP Activity Report 14(2007) 227; ibid 15 (2008) in these repot.
[5] C. Stock et el., arXiv:0712.0172v1.

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1-3-12

Correlation between ferromagnetism and superconductivity in UGe2
N. Aso, S. BanA , K. DeguchiA , T. FujiwaraB , Y. UwatokoC , N. K. SatoA
NSL-ISSP, Univ. of Tokyo, Graduate School of Sci., Nagoya Univ.A ,Graduate School of Sci. and Engineering, Yamaguchi Univ.B , ISSP, Univ. of TokyoC
Saxena et al.
discovered the ferromagnetic (FM) superconductor UGe2 inwhich superconductivity (SC) occurs at
high pressure range between ∼1.0 and ∼1.5 GPa. [1]. In the FM phase, there
seems to be another phase transition or
crossover at Tx ( 32 K at ambient pressure). This characteristic temperature Tx
also decreases with increasing P and becomes suppressed to zero at a critical pressure Px ( 1.2 GPa) where a maximum
SC transition temperature (TSC ∼ 0.7 K)
appears. In our previous work [2], we
presented the temperature dependence ofmagnetic Bragg peak intensities under P by
the neutron diffraction (ND) technique toreveal the nature of the transition at Px . We
have found that the low-T behavior of theuniform magnetization can be explainedby a conventional Stoner model, indicatingthat the FM state below Px can be understood as the perfectly polarized state.
Very recently, Ban et al. reinvestigateda SC phase diagram of UGe2 by AC magnetic susceptibility measurements. [3] They
found that the TSC and volume fraction
show a “M-shaped” structure as a functionof P and suggested that both of two critical points play an important role in the occurrence of SC. These observations are possibly ascribed to the improved homogeneity of the P transmitting medium. To examine the correlation between SC and FM
in UGe2 , we have to perform ND measurements by simultaneously detecting the superconductivity in UGe2 .
A single crystal was grown by Czochralsky pulling method with a tetra-arc furnace. The P was generated by a berylliumcopper pressure cell [4] using deutride
methanol and ethanol mixture as a P transmitting medium. [2, 4] Coils of ac susceptibility measurements are wound in the out-side of the cylinder as shown in ﬁg. 1. The
P was estimated by determining the TSC
of Sn. Elastic ND experiments has been
performed on the triple-axis spectrometer
PONTA (5G) at temperature down to 0.1 K
using a dilution refrigerator.
In this study, although the pressure wastuned just at Px , unfortunately only 20 %volume fraction of SC at 0.1 K were seen
with TSC ∼ 0.4 K in UGe2 . Furthermore wehave to tilt the dilution fridge by ∼ 4 degrees and then the outer coil may touch theradiation shield of the fridge. Thus we are
now analyzing the obtained neutron data.
References[1] S.S. Saxena et al., it Nature (London) 406,
587 (2000).
[2] N. Aso et al., Phys. Rev. B 73, 054512 (2006).
[3] S. Ban et al., J. Magn. Magn. Mater. 310,
e120 (2007).
[4] N. Aso et al., AIP Conf. Proc. 850 (2006) 705.

Fig. 1. Pressure cell together with the AC susceptibility coil.

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1-3-13Observation of magnetic form factor using detwinned single crystal of La2 CuO4
H. Kimura1 , T. Adachi1 , Y. Noda1 , M. Fujita2 and K. Yamada2
1 IMRAM, Tohoku University
2 IMR, Tohoku University
Fobs comparing the case of < j0 > form factor. The present result is consistent with theresults obtained from the magnetic form
factor in Nd2 CuO4 [2].
References[1] H. Ichikawa et al.: Physica B 281&282(2000) 482.
[2] H. Kimura et al.: Physica B 385&386 (2006)133.

La2CuO4 97 % detwinned(a) <j0>
4

Fobs

3

2

1

RF = 16.9 %0(b) dx2-y2 orbital
4

3

Fobs

Imaging of spin density distribution has
been tried to understand the 3d-electron
orbital state which contributes to a large
variety of physics in strongly correlated
electron systems. A polarized neutron
diffraction has been used for this trial
and clariﬁed the orbital order in ferromagnetic YTiO3 [1]. In the present study, we
performed crystal- and magnetic structure
analyses by using four-circle diffractometerwith unpolarized neutron to observe accurate magnetic form factor of 3d-electron orbital. The target material of this study is
La2 CuO4 (LCO). LCO is an antiferromagnet with 3d9 conﬁguration for Cu2+ ion andthus S = 1/2 spin should localize on d x2 −y2orbital.
The single crystal of LCO was grownby TSFZ method. The crystal was cut
and polished perpendicular to orthorhombic a-axis. The shaped crystal was heated
above structural phase transition temperature from orthorhombic to tetragonal phase
under uniaxial strain along a-axis to makethe detwinned crystal in the orthorombic
phase. As a result, we succeeded in obtaining 97 % detwinned single crystal of LCO.
The measurements were performed using
the four-circle diffractometer FONDER installed at T2−2 thermal guide in JRR-3M.
The wavelength of neutron was 1.243 Å.
The maximum values of sin θ/λ for magnetic Bragg reﬂections were about 0.6 Å−1 .
Crystal structure analysis was ﬁrstly performed to obtain the exact scale factor,
which was well solved with a reliability
factor of R = 4.2 %. The magnetic structurewith an assumption of < j0 > magnetic
form factor was solved with RM = 16.9 %.
On the contrary, as shown in Fig. 1, Fcalc
derived using the magnetic form factor ofd x2 −y2 orbital much better reproduces the21

RF = 8.9 %
0
0

1

2

3

4

Fcalc

Fig. 1. Fobs vs. Fcalc plot. Fcalc ’s are calculated using(a) isotropic < j0 > form factor and (b) anisotropic
d x2 −y2 orbital.

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JAEA-Review 2011-050

1-3-14

Relation between low-energy phonons and a charge stripe order inLa2−x Srx Cu1−y Fey O4
H. Kimura1 , Y. Ishikawa1 , Y. Noda1 , K. Enoki2 , M. Fujita2 and K. Yamada2
1 IMRAM, Tohoku University
2 IMR, Tohoku University
phonons down to T = 10 K and also no
anomaly around T = 55 K (≡ Tcharge ), below which the charge stripe order occurs.
This clearly shows that there is no structural phase transition below Tcharge and thesystem retains the LTO structure. On thecontrary, as shown in Fig. 1 (b), the linewidth in the phonon spectra starts narrowing below Tcharge , indicating that the life
time of phonons gets longer in the stripe ordered phase. More systematic studies are
required to clarify the relevance between
the charge stripe order and the narrowingof the phonon.

Phonon energyph (meV)

La1.87Sr0.13Cu0.99Fe0.01O4, Q = (1 0 4)
2.2(a) Phonon energy

2.0

1.8

1.6
0.8

(b) Line widthLine width (meV)

It is well known that the charge stripe
order in high-Tc cuprates competes withsuperconductivity. The previous neutron
and X-ray diffraction studies have shownthat the stripe order stabilizes only in
La-214 compounds in which the concentration of doped hole is the vicinity of
1/8 and the crystal structure is so-called
low-temperature tetragonal (LTT) or lowtemperature less orthorhombic (LTLO).
However, it was recently found in neutron
and X-ray diffraction study that the charge
stripe order is induced by substituting asmall amount of iron with a large magnetic
moment for copper, where the system is believed not to be the LTT or LTLO phase but
to be the low-temperature orthorhombic(LTO) phase. This is the ﬁrst discovery ofmagnetically induced charge stripe orderin the LTO phase. However, the origin of
this charge order is not clariﬁed yet. In thepresent study, we measured soft phonons
associated with the structural phase transition from the LTO to the LTT/LTLO, toconﬁrm whether the structural phase transition into LTT/LTLO phase really occurs.
ThesinglecrystalofLa2− x Srx Cu1−y Fey O4 with x = 0.13
and y = 0.01 (LSCFO) was grown by
TSFZ method. Inelastic neutron scattering
measurements for soft phonons were
performed at triple-axis spectrometer HER
installed at C1−1 cold neutron guide in
JRR-3M. The ﬁnal energy of neutrons was
ﬁxed at 4 meV with the energy resolutionof 0.2 meV.
Figure 1 (a) shows the energy of soft
phonons at Q = (1 0 4) as a functionof temperature. Although the phonon
becomes soft with decreasing temperature, there is no complete condensation of

0.6

0.4

Tcharge
0

20

40

60

80

100

Temperature (K)Fig. 1. Temperature dependences of (a) Phonon energy ωph and (b) Line width for (1 0 4) phonon.

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JAEA-Review 2011-050

1-3-15

Search for magnetic scattering in Fe and Pb co-doped Bi2201
H. Hiraka and K. Yamada
IMR, Tohoku University
There is no conclusion yet about the origin of attractive force that creates Cooper
pairs and eventually high-Tc superconductivity. Recent inelastic neutron scattering studies revealed that the so-called
hourglass-like magnetic dispersion relation commonly exists in La214 [1], Y123 [2],and Bi2212 [3] systems, thus indicating themagnetic interaction as a prime candidateof pairing mechanism. However, no magnetic cross section has been experimentally
reported yet in one of the most typicalcuprate superconductors, Bi2 Sr2 CuO6+δ
(Bi2201). So, we tried to ﬁnd magnetic
signals from this CuO2 mono-layer system
to establish universal features among highTc superconductors. Because Cu-site substitution enhances elastic and low-energy
neutron magnetic scattering in La214 system [4, 5], we doped Fe atoms in this study
by expecting a substantial impact on magnetic correlations due to its large magnetic
moment. In addition, Bi atoms were partially substituted by Pb atoms, so that large
single crystals (∼cm-size in length) could
be easily grown by TSFZ techniques.
Neutronscatteringexperiments
were carried out on triple-axis spectrometers
AKANE
and
TOPAN
using as-grown single crystals of=0,Bi1.74 Pb0.38 Sr1.88 Cu1−y Fey O6+δ (y0.01, 0.03, and 0.05). Figure 1 shows acontour map of intensity difference ofelastic scattering between 3 K and 300 K,
measured on AKANE under the triple-axis
mode using 3%-Fe doped sample around(1, 0, 0)ortho , or (π, π). A pair of broad
peaks is clearly seen at (0.8, ±0.2, 0)ortho , inaddition to the nuclear peak at (1, 0, 0)ortho .
Later on, another pair was conﬁrmed at(1.2, ±0.2, 0)ortho , and the same four-foldstructure was observed in (3, 0, 0)ortho zone
with weak intensity. The onset temperature of this diffuse scattering (∼30 K)

is comparable to that in spin-glasses ofLa214 [6]. These facts strongly support
that this symmetric cross section has themagnetic origin. (Indeed, we conﬁrmed itby polarized neutron experiments.) Thismagnetic scattering is incommensurate
and similar to that in La214 system, except
the large incommensurability (δ ∼ 0.20).
We conjecture that Fe spins may reﬂect
underlying magnetic modulations in pure
Bi2201 system. Search for the dynamicalmagnetic component is now in progress.
References[1] J.M. Tranquada et al., Nature 429, 524(2004).
[2] C. Stock et al., Phys. Rev. B 71, 024522(2005).
[3] B. Fauque et al., cond-mat/0701052.
[4] K. Hirota et al., Phys. B 241-243, 817 (1998).
[5] H. Hiraka et al., Phys. C 408-410, 775(2004).
[6] S. Wakimoto et al., Phys. Rev. B 60, R769
(1999).
Bi2201+Fe(3%), As-grown sample-C, (h, k, 0)ortho
AKANE, 20Ei, g-open-120'(taper)-B, 3-axis, flat-A, 1D
E = 0 meV, I(3K) - I(300K)

Net intensity/ 400 mon.~ 4.8 min

0.4

140

0.2
100

k

0

60

-0.2

-0.4

20
0.6

0.8

1

1.2

1.4

h

Fig. 1. Contour map of intensity difference of elastic
scattering between 3 K and 300 K.

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JAEA-Review 2011-050

1-3-16
Magnetic Correlation in the Kondo-Semiconductor-like Material CeOs4 Sb12
K. Iwasa1 , S. Itobe1 , M. Kohgi2 , C. Yang1 , K. Kuwahara2 , H. Sugawara3 , H. Sato2 , N.
Aso4
1
Tohoku Univ. , Tokyo Metropolitan Univ.2 , The Univ. of Tokushima3 , Univ. of Tokyo4
romagetic ordering in the low ﬁeld region
to the metallic one above 1 T without theantiferromagnetic state. We have tried to
identify an order parameter in the higher
magnetic ﬁeld region above 1 T, and carriedout the polarized neutron diffraction using PONTA (5G) and TOPAN (6G). The observed ﬂipping ratio intensities were transformed into the magnetic form factor, as
shown in Fig. 1. Although the data points
scatter owing to low statistics from thetiny magnetic moment even under magnetic moment, the overall feature against
the scattering vector coincides with the calculated one for Ce3+ based on the dipole
approximation shown by the solid line. No
clear change was seen in the form factor
across the phase boundary, thus the magnetic moment distribution has no trace ofthe ordering nature. We will continue themeasurement to reveal the order parameterin the high magnetic ﬁeld region.

Magnetic form factor [ B / f.u.]

0.3

0.2

m

CeOs4 Sb12 has been considered as a
Kondo semiconductor characterized by aband gap of around 10 K estimated fromthe temperature dependence of electrical resistivity, while it shows the large
T-linear coefﬁcient of speciﬁc heat γ =200 mJ/K2 /mol (E. Bauer et al.: J. Phys.:
Condens. Matter 13 (2001) 4495, H. Sugawara et al.: Phys. Rev. B 71 (2005) 125127).
Previous inelastic neutron scattering experiment revealed no clear crystal ﬁled excitation, in contrast to the Curie-Weiss behavior of magnetic susceptibility above 100?K(C. P. Yang et al.: J. Phys. Soc. Jpn. 74(2005) 2862). It is notable that this material shows a phase transition at 0.9 K under zero magnetic ﬁeld and the ordering
temperature is enhanced by applied magnetic ﬁelds. The low-temperature magnetic
instability is expected to be a formation ofspin density wave (SDW) by the enhanced
density of state at the Fermi level undermagnetic ﬁeld, as discussed in the theoretical arguments based on the periodic Anderson model (T. Ohashi et al.: Phys. Rev. B
70 (2004) 245104).
We performed neutron diffraction experiment using the triple-axis spectrometers
TOPAN (6G) and HER (C1-1) and the dilution refrigerator of ISSP, Univ. of Tokyo.
We succeeded in observing weak antiferromagnetic reﬂections characterized by thewave vector q = (1 0 0) below the ordering temperature. Assuming the magnetic
ordering at the Ce-ion sites forming thebcc lattice, we evaluated the ordered moment magnitude of (0.07 ± 0.02)μB /Ce thatis consistent with the SDW scenario. On
the other hand, the antiferromagnetic peak
disappears above 1 T in contrast to the reported enhancement of the transition temperature. The electronic state changes fromthe less-conductive state with the antifer-

0.1

0.0

CeOs4Sb12
B = 5 T // [0 0 1]
T = 37 mK-0.1
T = 4.5 K
calculated
0.0
0.2
0.4

0.6

0.8

sinq / l [Å ]-1Fig. 1. Magnetic form factors of CeOs4 Sb12 at 5 T.

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JAEA-Review 2011-050

1-3-17Visualization of rattling in ﬁlled skutterudite compounds
K. Kaneko A , N. Metoki A,B , H. KimuraC , Y. NodaC , T. D. Matsuda A , M. KohgiD
A Advanced Science Research Center, Japan Atomic Energy Agency
B Department of Physics, Tohoku University
C Institute of Multidisciplinary Research for Advanced Materials, Tohoku University
D Department of Physics, Tokyo Metropolitan University
Filled skutterudite compounds LnT4 X12
where Ln is rare earth, T is transition metal
and X is pnictogen, exhibit wide variety ofphysical properties by combination of Ln,
T and X. Recently, large thermal vibration of a rare earth ion, so-called ratting,becomes one of the key issue as a possible
origin of interesting physical properties including unconventional heavy-fermion superconductivity in PrOs4 Sb12 , Nd-based
heavy-fermion behavior in NdOs4 Sb12 andso on. In order to reveal detailed picturesof the rattling and its relationship with f electron, single crystal neutron diffraction
experiments on PrOs4 Sb12 and NdOs4 Sb12
were carried out on 4-circle diffractometer
FONDER. The maximum entropy method
is employed in the structural analysis to
avoid arbitrariness, which was achieved
using software PRIMA and VESTA.
Figure 1 shows obtained nuclear scattering length density (hereafter, nuclear
density) distributions of PrOs4 Sb12 andNdOs4 Sb12 at room temperature. These
results correspond to the space- and time
averaged nuclear density reﬂecting thermal vibration. Taking into account the difference in the coherent scattering length
between Pr and Nd, bPr =4.58 fm andbNd =7.69 fm, isosurface levels in Fig. 1
are set at 4.58 fm/Å3 and 7.69 fm/Å3
for(a) PrOs4 Sb12 and (b) NdOs4 Sb12 , respectively.
Widely spread nuclear density distributions could be seen at the center of the cage,corresponding to Pr and Nd. Note that theshapes for both Pr and Nd are not spherical, namely, both ions exhibit anisotropic
thermal motion. A contrast between Pr and
Nd is found in anisotropy and magnitudeof spatial extent. In PrOs4 Sb12 , the dis-tribution of Pr has an almost cubic shapewith the edge parallel to the 100 direction
and the width is broadest along the 111
direction. The spatial extent of Nd distribution in NdOs4 Sb12 is wider than thatof Pr, and becomes rather isotropic. The
width along the 100 direction is slightly
larger than that along 111 in NdOs4 Sb12 ,which is contrary to PrOs4 Sb12 . It should
be pointed out that both 100 and 111
directions for Ln ion correspond to thevoids of the Sb icosahedron cage. In contrast, the nuclear distribution of Os and Sb
in PrOs4 Sb12 quite resembles to those in
NdOs4 Sb12 . Further diffraction studies on
detailed temperature dependence and extension to LaOs4 Sb12 could provide keen
insights on anisotropy with regard to a roleof 4 f electron and its relationship to various physical properties.

Fig. 1. Nuclear density distributions of PrOs4 Sb12
and NdOs4 Sb12 at room temperature.

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JAEA-Review 2011-050

1-3-18Magnetic Excitation of Ferromagnetic System NdFe4 P12 Exhibiting Heavy
Electron Behavior
K. Iwasa1 , L. Hao1 , K. Saito1 , H. Sugawara2 , H. Sato3
Tohoku Univ.1 , The Univ. of Tokushima2 , Tokyo Metropolitan Univ.3
romagnetic ordered state, and no distinct
dispersion relation is detected near the ferromagnetic zone center Q = (1 1 0). It is
indicative that the magnetic excitation has
energy gap of 1 meV, which may come fromthe anisotropy of crystal ﬁeld. The magnetic excitation is consistent with the ferromagnetic ordering, so that the anomalous
behavior of NdFe4 P12 can not simply be attributed to the magnetic Kondo effect.

Counts / 1000 kMN

1200
160 Q = (0.85 0.85 0)
0.7 K
140
3.0 K
120

1000
800

100
80

600

60

400

40
200

20
0
-2

Counts / 100 kMN

In the study of strongly correlated electron phenomena of rare-earth ﬁlled skutterudite compounds, heavy electron statein the system having two or more 4 f electrons per rare-earth ion has been a topic.
PrFe4 P12 with 4 f 2 conﬁguration of Pr3+ is atypical system, which shows the Sommerfeld coefﬁcient for electronic speciﬁc heatγ = 1.4 J/mol/K2 and the clear -logT behavior of electrical resistivity (Y. Aoki etal.: Phys. Rev. B 65 (2002) 064446, H.
Sugawara et al.: Phys. Rev. B 65 (2002)
134411). Our inelastic neutron scatteringexperiment revealed the quasielastic magnetic response indicating the strongly hybridized state (K. Iwasa et al.: Acta Physica Polonica B 34 (2003) 1117). A similar− logT behavior is also found in NdFe4 P12with 4 f 3 conﬁguration of Nd3+ (H. Sato etal.: Phys. Rev. B 62 (2000) 15125). However,it undergoes a ferromagnetic phase transition at TC = 1.9 K and the magnitude of ordered magnetic moment was evaluated as
1.6μB/Nd (L. Keller et al.: J. Alloys and Compounds 323-324 (2001) 516), which is muchlarger than the typical heavy electron materials and seems not to be consistent withthe singlet formation due to Kondo effect.
Thus, the heavy electron behavior in electrical resistivity of NdFe4 P12 together withwell localized 4 f electrons is a mysterious
property. In order to investigate the 4 f electron state of this material, we performed inelastic neutron scattering experiments. The
triple-axis spectrometers TOPAN (6G) andHER (C1-1) were used to measure energy
spectra from a single-crystalline sample.
Figure 1 shows energy spectra at Q =(0.85 0.85 0) of NdFe4 P12 at 0.7 and 3 Kabove and below TC , respectively. We observed a peak at 1 meV at 0.7 K and it disappears at 3 K above TC . This peak can be
assigned to a collective excitation in the fer-

-1

0

1

2

0

Energy [meV]Fig. 1. Energy spectra at Q = (0.85 0.85 0) of
NdFe4 P12 at 0.7 and 3 K.

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JAEA-Review 2011-050

1-3-19Crystal-ﬁeld excitation in Pr(Ru1−x Rhx )4 P12
K. Iwasa1 , K. Saito1 , L. Hao1 , Y. Murakami1
Tohoku Univ.1
sample appears, which is not observed in
the x = 0 sample. The 2.4 meV peak iscommon for the Rh doped samples, and theexcitation energy does not depend on temperature. Moreover, the integrated intensity increases with the increment of the Rh
concentration. The Rh doping modiﬁes the
Pr 4 f crystal-ﬁeld levels not to shift against
temperature variation, then the hexadecapolar ordering with the level shifts is suppressed. An additional 4d electron of Rh
is expected to be doped in the conduction
band. The metal-nonmetal transition of
PrRu4 P12 is sensitive not only to the p state
originating from the pnictogen P but also to
the 4d state by the transition-metal site.

Counts / 750 kMN (~300 sec)

200

6000
Q = 1.5 [2π/a]
T=7K
x = 0.03
x=0

150

5000
4000

100

3000
2000

50
1000
0
-2

0

2

4

6

Counts / 100 kMN (~40 sec)

Higher-rank multipolar ordering of 4 felectron state of Pr-ﬁlled skutterudite has
been a fascinating topic. PrRu4 P12 is atypical system, in which the antiferro-type
hexadecapolar (rank-4 multipolar) ordering occurs below the metal-nonmetal transition at 63 K. This phase transition is interpreted as a new type of charge density
wave formation due to the Fermi surface
nesting property strongly coupled with themodulated 4 f multipolar arrangement. p- f
hybridization between 4 f and conduction
electrons plays an essential role in the ordering mechanism. However, some properties have remained unsolved. The lowtemperature resistivity does not diverge
with decrease of temperature, and the nonmetallic state is easily suppressed by magnetic ﬁeld of 1 T. The weak nonmetallic
state is expected to originate from othermechanism in addition to p- f hybridization. The substitution of Rh to Ru gives rise
to rapid suppress of metal-nonmetal transition; the electrical resistivity at low temperature in the Rh 10% system becomes thesame magnitude at around 60 K. Thus, thedoping effect is a key to understand theweak nonmetallic phase of PrRu4 P12 . Then
we have carried out inelastic scattering experiments to measure crystal-ﬁeld excitation of Pr(Ru1− x Rhx )4 P12 .
We performed the experiments using thetriple-axis spectrometers HER (C1-1) and
TOPAN (6G) for polycrystalline sample ofPr(Ru1− x Rhx )4 P12 (x = 0, 0.03, 0.05, 0.10 and0.15). Figure 1 depicts the low-energy spectra of the samples of x=0 and 0.03 at 7 K.
The peak at 3.2 meV of the x = 0 sample corresponds to the exitation from the(2)ground state triplet Γ4 to the ﬁrst excitedstate singlet Γ1 , which exhibit strong temperature dependence below the transition
temperature. On the other hand, a strong
peak at 2.4 meV in the data of the x = 0.03

0Energy [meV]Fig. 1. Crystal-ﬁeld excitations of PrRu4 P12 andPr(Ru0.97 Rh0.03 )4 P12 at 7 K.

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JAEA-Review 2011-050

1-3-20Spin-lattice dynamics in rare earth antiferroquadrupolar ordering conpound
HoB2C2
K. Ohoyama , H. Onodera(A), E. Matsuoka(A)IMR, Tohoku Univ., Faculty Science, Tohoku Univ.(A)lations from the (100) to (101/2) reciprocal
position at T=1.56K observed on C1-1. We
found two magnetic modes at about 3meVand 0.8meV at the zone centre (100). The
lower excitation shows obvious dispersion,
while the dispersion of the higher mode isrelatively weak. We also observed dispersion relations along the a*-direction.
From the temperature dependence ofthe magnetic excitation spectra, we conﬁrmed that the lower mode becomes weaknear the transition temperatures, and disappears above the transition temperatures,indicating that the lower dispersive modeis important for the AFQ and AFM ordering in HoB2C2.
References[1] H. Yamauchi et al.: J. Phys. Soc. Jpn. 68(1999) 2057.
[2] H. Onodera et al.: J. Phys. Soc. Jpn. 68(1999) 2526..
[3] A. Tobo et al.: Physica B 312-313 (2002)
853-854.
HoB2C2 Dispersion along c* at T=1.56K
4

Excitation Energy (meV)The RB2C2 (R=rare earth) compounds,
which have the tetragonal LaB2C2 typestructure with P4/mbm symmetry, show
diversiﬁed magnetic properties caused bycoexistence of antiferroquadrupolar (AFQ)
and antiferromagnetic (AFM) interactions.
In particular, DyB2C2 is the ﬁrst tetragonal rare earth compound in which an
AFQ ordering is realised. Since the exact
ground state by crystalline electric ﬁeld under tetragonal symmetry has no degree of
freedom on electric quadrupolar moments,
it was thought that no AFQ ordering canbe realised in the tetragonal rare earth compounds.
On the contrary, we have proved thatsome of RB2C2 are AFQ ordering compounds with higher TQ than other typical AFQ compounds. Thus, to understand necessary conditions of AFQ orderings in rare earth compounds, it is indispensable to clarify characters of the AFQ
ordering in RB2C2. Of the RB2C2 system,
HoB2C2 is particularly unique because of
the following points: (i) the AFQ ordering in HoB2C2 is realised at TQ=4.5K below the magnetic ordering temperature,
TN=5.9K[2], (ii) anomalous magnetic diffuse scattering is observed above TQ up to2TQ[3].
To understand the magnetic properties
of HoB2C2 around the transition temperatures, we think clarifying spin-latticedynamics is indispensable because magnetism and lattice is strongly coupledthough the strong LS coupling. Therefore,
we performed inelastic scattering experiments to observe higher energy excitations
on 6G, and low-energy excitations on C11. In 2007, we succeeded in observing dispersion relations of some modes of magnetic excitations below 4meV in the ordered state. Figure 1 shows dispersion re-

3

2

1

0

-0.1

0.0
(1,0,0)

0.1

0.2
0.3
(1, 0 ,L)

0.4

0.5
(1,0,0.5)

Fig. 1. Dispersion of magnetic excitations along thec* direction in HoB2C2 at T=1.56K

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1-3-21

Coexistence of superconductivity and magnetism in a multi-layered cuprate
C. H. Lee(A), A. Iyo(A), K. Kihou(A), H. Kito(A) and K. Yamada(B)(A) AIST, (B) IMR Tohoku Univ.
One of the most signiﬁcant feature inhigh-Tc cuprates is that superconductivity
is inextricably linked with antiferromagnetism. Crucial issue for understanding
the mechanism of cooper pairs formation iswhether the same carrier is responsible forboth magnetic long range ordering and superconductivity. Recently, NMR and uSRmeasurements show that antiferromagnetism exists in superconducting phaseof multilayered cuprates. In particular,
NMR measurements suggest that antiferromagnetism coexists with superconductivity microscopically on a single CuO2 planein underdoped HgBa2Ca4Cu5O12+d. Experiments using diffraction technique arehighly required to clarify whether it is along range ordering or not.
Neutron scattering measurements werecarried out using a powder diffractometer, HERMES, and a triple-axis spectrometer, AKANE, at the JRR-3 reactor of JAEA
at Tokai. On the experiments with HERMES, the incident neutron wavelength was
ﬁxed at 1.8265 A using (311) reﬂection of
the Ge monochromator. The sequencesof horizontal collimators were 12’-blankS-22’ where S denotes the sample position. On the other hand, on the expermiments with AKANE, the incident neutron wavelength was ﬁxed at 2.044 A using a pyrolytic graphite (PG) monochromator. The sequences of horizontal collimators were 12’-blank-S-15’. Powder of
HgBa2Ca4Cu5O12+d was used as a sample.
Fig. 1 shows spectra of theta-2theta scanin HgBa2Ca4Cu5O12+d sample at T=12K
and 300K. A peak around 2theta = 15.7 at
T = 12K is also observed at T=300K, indicating that the peak include a fundamental
nuclear peak of (003) or even some impurity phases. Even if magnetic component
exists, the intensity should be quite small

comparing to the observed peak intensity.
A solid line depicts calculated spectra assuming magnetic moment of Cu atoms on
inner CuO2 plane as 0.67uB estimated by
NMR measurements. Clearly, such a welldeﬁned magnetic peak is not observed, indicating that the magnetic moment should
be quite small. We also checked that welldeﬁned magnetic peak is not observable ina wide 2theta region.

Fig. 1.
Spectra of theta-2theta scan in
HgBa2Ca4Cu5O12+d at T=12K and 300K.
A
solid line depict the result of simulation assuming
0.67 uB as magnetic moment of Cu atoms on inner
CuO2 plane.

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JAEA-Review 2011-050

1-3-22Flux line lattice in ErNi2 B2 C

H. Kawano-Furukawa, R. Nagatomo, S. Konno, S. Ohira-Kawamura,H.
H. Yoshizawa
Yoshizawaaa andandb
H. Takeya
Ochanomizu Univ., ISSP NSL Univ. of Tokyoa and NIMSb
In ferromagnetic superconductors, an internal magnetic ﬁeld Hint mediated by theferromagnetic moments may lead a spontaneous vortex phase [1,2,3]. But there is noexperimental report for a realization of thephase so far.
ErNi2 B2 C (Tc ∼ 10.5 K, TN ∼ 6 K, TWFM
∼ 2.3 K) is one of possible candidates forthe spontaneous vortex phase, because Hc1of the system shows an abrupt decrease below TWFM and it seems to become zero ataround 1.8K, which satisﬁes the conditionof the spontaneous vortex phase [4,5,6,7].
To check this possibility, we started to
study the ﬂux line lattice on ErNi2 B2 C bya small angle neutron scattering (SANS)
technique.
In this study, we used un-anealed single
crystals of ErNi11
2 B2 C (Tc ∼ 8.6 K) grownby a ﬂoating zone method. The SANS experiments were performed at the SANS-U
spectrometer in JRR-3, JAERI, Japan. External ﬁelds Hext were applied parallel to boththe crystallographic b axis and the incident
neutron beam. Neutrons with wavelength
λn = 11 Å were selected by a velocity selector, and an area detector at the end of a 16 mlong evacuated chamber counted neutrons
scattered by the FLL. To maximize neutrontransmissions the sample were cut with 1
mm thickness along the neutron beam.
Figures show temperature dependenceof FLL diffraction patterns observed under
Hext = 6400 Oe. The upper panels show
data measured after ﬁeld cooled processes(FC) but the bottom ones were recorded
after ﬁeld cooled and oscillated processes(FCO). Down to 4K, all ﬁgures show rhombic FLL patterns. However, at lower temperatures, these two processes give different results. Namely, the FLL patterns after
the FC processes remain the rhombic FLL
but those after the FCO processes show cu-

bic one. From this result, we lead two conclusions: (1) the rhombic FLL in FC process
is due to vortex pinning and (2) an oscillation ﬁeld of 800 Oe is enough to release thevortex pinning. From the present study, we
succeeded in construction of a phase diagram of the FLL structure on ErNi11
2 B2 C.
We are on the process to verify the spontaneous vortex phase in this compoundand the further experiments are planed.
[1] E. I. Blount et al., Phys. Rev. Lett. 42,
1079 (1979).
[2] M. Tachiki et al., Solid State Commun.
31, 927 (1979); ibid. 34, 19 (1980).
[3] H. S. Greenside et al., Phys. Rev. Lett.
46, 49 (1981).
[4] H. Kawano et al., J. Phys. Chem.
Solids 60, 1053 (1999).
[5] T. K. Ng et al., Phys. Rev. Lett. 78, 330(1997).
[6] H. Kawano-Furukawa et al., in Rare
Earth Transition Metal Borocarbides (Nitrides): Superconducting, Magnetic andNormal State Properties, Vol. 14 of NATOadvanced Study Institute, Series II, editedby K. H. Muller and V. Narozhnyi (Kluwer
Academic, Dordrecht, 2001), p. 223.
[7] Mariko V. Jarić, Phys. Rev. B 20, 4486
(1979).

Fig. 1. Temperature dependence of FLL patterns after FC and FCO processes.

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1-3-23Magnetic and electronic nature of metallic ferromagnet Sn2Co3S2 and its related
compounds
M. Matoba, A. Umetani, E. Nagoshi, S. Nakajima, and T. Kubodera
Center for Applied Physics and Physico-Informatics, Keio University, 3-14-1 Hiyoshi,
Yokohama 223-8522
Pyrite- and shandite-type Co disulﬁdesare both mineral-related materials that canbe artiﬁcially synthesized. Pyrite-type ferromagnetic CoS2 (TC=120K) and its related
compounds have been the subject of theintense research because of their variety
of interesting physical properties [1] to reveal their correlated electron nature. On theother hand, few studies have been madeof shandite-type ferromagnetic Sn2Co3S2(TC=177K) [2-4].
Recently, crystallographic and electronic structure effects in (Sn,In)2Co3S2
has been investigated by X-ray diffraction(XRD) and local spin density approximation (LSDA) band calculations to discuss its
structural nature from the viewpoint of thehalf antiperovskite (SnCo3/2S) [3]. However, electronic and magnetic properties of
Sn2Co3S2 has not been examined in detailbeyond LSDA and the electronic bonding
nature is not clear. In this paper, we report the hitherto unknown magnetic andelectronic nature of shandite-type A2Co3S2(A=Sn, In) as the strong correlated electron
system (SCES).
Polycrystalline A2Co3S2 (A=Sn, In) samples were carefully prepared by a solidstate reaction method in a evacuated quartz
tube [4]. Obtained samples were characterized by powder XRD, powder neutron
diffraction (PND) by the high efﬁciency
and high resolution measurements (HERMES) [5], and Rietveld analysis using the
programs Rietan2000 and PRIMA [6]. The
electronic and magnetic nature were analysed by XPS spectro- and SQUID magnetometers, and the electronic structure of
Sn2Co3S2 was calculated by LSDA+U
method (the LMTART code [7]).
Figure 1 (top-left panel) displays Co
2p core-level XPS spectra of Sn2Co3S2 incomparisson with those of reference compounds [8-10]. One can see that each ofspin-orbit components (2p3/2 and 2p1/2
peaks) indeed shows a strong satellitefeature at higher binding energy side of
the main peak. Co 2p XPS spectrum of
Sn2Co3S2 exhibits a complicated feature,and it can be considered as the spectrumwith two shape components by XPS peak
shape analysis. In the top-left panel ofFig.1, the solid curve (a) is the total estimated spectrum with two shape components (curves (b) and (c)), demonstrating
the very good agreement between experimental and calculated spectra of Sn2Co3S2.
The shape of component (b) is similar tomain peak shapes of Co and TlCo2S2; theshape of component (c) resembles the satellite shape of TlCo2S2, and is quite similar to that of strongly correlated Co compound K2CoF4. These feature might contain some information on the Co-Sn/CoS bonding nature and the electron correlation in Sn2Co3S2. Thus, the effects of metallic Co-Sn and inoic/covalent Co-S bondings are considered to be seen as the complicated feature in the Co 2p XPS spectra. This is indeed similar to the situation in ThCr2Si2-type TlCo2S2 indicatingthat the effect of Co-S bonding is seen as
satellite structures in the Co 2p XPS spectra [10]. We therefore analyzed the spectrum by the conﬁguration interaction cluster model [8] to estimate the on-site d-d
Coulomb repulsion energy U=4 eV, indicating that the electronic nature of the Co3S2
units in Sn2Co3S2 belongs to SCES.
The bond-valence-sum (BVS) calculation[11] was carried out to evaluate the valence state of the Co ions (formal charge of
Co is 1.14) indicating that Co atoms havemixed valence; the ratio (Coˆ{0+}:Coˆ{2+})Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

is roughly 1:2. The mixed valence like complicated feature of Co 2p XPS spectrum of
Sn2Co3S2 would be explained by two different metallic Co-Sn and ionic/covalent
Co-S bondings. Figure 1 (bottom panel) dispalys electron-density maps obtained by
maximum entropy method (MEM)-based
whole pattern ﬁtting and LSDA+U calculation to suggest the layered structural nature and reveal that electron density at thesaddle point in Co-S bond is indeed threetimes larger than those of Co-Sn bonds,
indicating the difference of Co-Sn/Co-S
bonding nature and supporting the BVS result.
Finally, we would like to comment theelectronic nature of (Sn,In)2Co3S2 in which
TC is gradually decreased with x to be
zero at x=1. Fig.1 (top-right panel) showsmagnetic susceptibilities and electrical resistivities of (Sn,In)2Co3S2. Interestingly,
Rietveld reﬁnement of XRD and PND indicates that Sn atoms on the Sn1(3a) site
are regioselectively substituted by In atoms
for Sn2Co3S2. Furthermore, the ferromagnetic metal to pseudo-gap semiconductortransition is indeed observed at x=1 in(Sn,In)2Co3S2. Further experimental andtheoretical studies of the spin, charge andorbital degrees of freedom for Sn2Co3S2 asSCES would be of great interest, and the socalled chemical tuning research is now inprogress.
References[1] S. Ogawa, J. Appl. Phys. 50, 2308 (1979).
[2] S. Natarajan et al., J. Less. Common.
Metals. 138, 215 (1988).
[3] R. Weihrich and I. Anusca, Z. Anorg.
Allg. Chem. 632, 1531 (2006).
[4] T. Kubodera et al., Physica B 378-380,
1142 (2006).
[5] K. Ohoyama et al., Jpn. J. Appl. Phys. 37,
3319 (1998).
[6] F. Izumi and T. Ikeda, Mater. Sci. Forum,
321-324, 198 (2000).
[7] S. Y. Savrasov, Z. Kristallogr. 220, 555(2005).
[8] A. Fujimori et al., J. Electron. Spectrosc.
Relat. Phenom. 62, 141 (1993).

[9] L. Sangaletti, F. Parmigiani, and E. Ratner, Phys. Rev. B 57, 10175 (1998).
[10] M. V. Yablonskikh et al., J. Phys. Condens. Matter 18, 1757 (2006).
[11] J. L. Tallon, Physica C 168, 85 (1990).

Fig. 1. (Top) Co 2p XPS spectra, magnetic susceptibilities, electrical resistivities, and (bottom) electrondensity maps in (100) and (110) planes of Sn2Co3S2.

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JAEA-Review 2011-050

1-3-24Charge and spin ordering in La1.85Ca0.15CoO4.17
K. Horigane, H. Haruhiro*, K. Yamada* and J. Akimitsu
Department of Physics and Mathematics, Aoyama-Gakuin University, Sagamihara 229-8558;*Institute for Materials Research, Tohoku University, Sendai 980-8577
strong intensity at L=half-integer. This result indicates that type-1 stacking domain
is dominant in a lower doping range, suggesting that the magnetic domains arechanged by Ca concentration around x=0.5.
To understand the relationship, we should
study other cobaltates which are substituted at A-site with various rare-earth andalkaline earth metals.

Intensity [counts/80kmon.]

Reference[1] K. Horigane et al.: JPSJ 76 (2007) 114715.
8000 (a) charge ordering
B-sap-30'-60'-B

6000
4000
2000
0

0

3500
Intensity [counts/80kmon.]In the neutron scattering experiments oflayered cobaltate, we studied the holedoping dependence of the charge andmagnetic orderings[1]. Charge order peaks
were insensitive to x, while the magnetic
diffraction pattern changed dramaticallybelow and above x=0.5. The type-1 reﬂections arised below x=0.5, whereas it
switches to the type-2 reﬂections avobe
x=0.5. From these results, we found thatthe type-1 and 2 stacking domains werechanged by Ca doncentration or Covalence. However, it is not straightforward
to understand the origin of magnetic structure by Ca doping. In order to understand the essence for magnetic domains inthis system, we examined the charge andmagnetic ordering in excess oxygen system
La1.85Ca0.15CoO4.17, of which cobalt valence is about Co2.5+.
Single crystal of La1.85Sr0.15CoO4.17 wasgrown by the TSFZ method, of which volume was about 1.0 cc. It was mounted in arefrigerator with the b-axis vertical, allowing to observe the (h,0,L) reciprocal latticeplane. To index the superlattice peaks, weuse a unit cell with dimensions √ 2a ×√
2a × c. The neutron scattering experiments
were carried out on the 3-axis spectrometer
TOPAN(6G). The incident neutron energy
was ﬁxed to be Ei=30.5meV, typecally witha sequence of collimation of blank-30’-60’blank.
Figure 1-(a) shows the charge order spectrum of (1,0,L). An integer-peak structure
was clearly observed, and it is consistent
with the checkerboard-type charge orderin La1.5Ca0.5CoO4. If the Ca concentration is essential for magnetic domains, it
is expected that magnetic peaks due totype-1 stacking are only observed. Figure 1-(b) shows the magnetic scatteringin La1.85Ca0.15CoO4.17. We observed the

1

2

3
4
5
L in (1,0,L)

6

7

8

magnetic ordering
B-sap-30'-60'-B

(b)

3000
2500
2000
1500
1000
500
0

0

1

2

3
4
5
L in (0.5,0,L)

6

7

8

Fig. 1.
(a)Structural scattering due tocheckerboard charge order at (1, 0, L) in
La1.85Ca0.15CoO4.17. The arrow indicate aluminum scattering. (b)Magnetic peaks at (0.5, 0, L)
in La1.85Ca0.15CoO4.17.

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1-3-25
Lattice eﬀects on the charge-spin ordering in layered cobaltates R1.5Sr0.5CoO4
K. Horigane, H. Haruhiro*, K. Yamada* and J. Akimitsu
Department of Physics and Mathematics, Aoyama-Gakuin University, Sagamihara 229-8558;*Institute for Materials Research, Tohoku University, Sendai 980-8577
system was very small. This result indicatethat A site radius, which corresponds tobandwidth, is coupled with the charge order in layered cobaltates.
Magnetic scatterings at q=(0.5, 0, L) in
Nd1.5Sr0.5CoO4 is shown in Fig.1-(b). We
observed scatterings with L=odd, and thisresult is same as that of LSCO system. Contrary to the case of charge ordering, magnetic ordering is hardly coupled with A site
radius.
Reference[1] I. A. Zaliznyak et al.: PRL 85 (2000) 4353.
[2] K. Horigane et al.: JPSJ 76 (2007) 114715.

500

Al(200)(a) g-open-B-B
Q=(1,0,L)
T=10K

600

Al(111)

Intensity [counts/60kmon.]

700

400
300
200
La Sr CoO

100

1.5

0.5

4

Nd Sr CoO
1.5

0

0

1

2

3
4
L in (1,0,L)

5

0.5

6

4

7

450
g-open-B-B
Q=(0.5,0,L)
T=10K

(b)
Intensity [counts/60kmon.]Layered transition metal oxides have beenmuch attention due to their wide variety ofmagnetic, electrical and structural properties. In some of the doped transition metalcompounds, there is a real space ordering
due to the charge carriers in a certain carrier concentration, resulting in an orbital
ordering (OO) and sometimes a charge ordering (CO). In a recent neutron scattering study, Zaliznyak el al. investigated ashort ranged checkerboard charge orderof Co2+/Co3+ (ξ co=23 Å) and magnetic
order at L=odd in the half-doped cobaltate La1.5Sr0.5CoO4 (LSCO:rA=1.19 Å) [1].
More recently, we performed neutron scattering experiments on La1.5Ca0.5CoO4(LCCO: rA=1.15 Å) [2]. Comparing the results between LSCO and LCCO systems,
we found that long-ranged checkerbord
charge order (ξ co(Ca)=115 Å) and new
type of magnetic reﬂections at L=halfinteger were observed in LCCO system.
Our purpose of this study is to clarify
the relationship between A site radius, rA,
and charge-spin ordering. Thus, we studied about charge and magneic orderings
in Nd1.5Sr0.5CoO4(NSCO: rA=1.16 Å) system.
Single crystal of Nd1.5Sr0.5CoO4 wasgrown by the TSFZ method, of which volume was about 1.0 cc. It was mounted in arefrigerator with the b-axis vertical, allowing to observe the (h,0,L) reciprocal lattice
To index the superlattice peaks,
plane.
we use a unit cell with dimensions √ 2a
×√ 2a × c. The neutron scattering experiments were carried out on the 3-axis spectrometer AKANE(T1-2).
Figure 1-(a) shows structural scatterings
due to checkerboard charge ordering of
R1.5Sr0.5CoO4 (R=La, Nd) in (1, 0, L). We
observed the scatterings with L=integer in
Nd system, while those of intensity in La

400
350
300
250
200
150

T=12K
T=60K
0

1

2

3
4
5
L in (0.5, 0, L)

6

7

8

Fig. 1. (a)Structural scattering due to checkerboard
charge order at (1, 0, L) in R1.5Sr0.5CoO4. The
arrows indicate aluminum scattering. (b)Magnetic
peaks at (0.5, 0, L) in Nd1.5Sr0.5CoO4.

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1-3-26

Cycloidal Spin Order in (Gd,Tb)MnO3 with Electric Polarization along the a-Axis
H. Sagayama(A), N. Abe(A), K. Taniguchi(A), T. Arima(A), Y. Noda(A), M. Soda(B), M.
Matsuura(B), K. Hirota(B), Y. Yamasaki(C), D. Okuyama(D), Y. Tokura(C,D)(A)IMRAM, Tohoku Univ., (B)ISSP, Univ. Tokyo, (C)Dept. Appl. Phys., Univ. Tokyo,(D)ERATO-MF, JST
In a orthorhombically distorted perovskite TbMnO3 , ferroelectric polarization
appears along the c axis below TC ∼27 K. The polarization ﬂops by 90 degrees to the a direction by the application of a magnetic ﬁeld along the b or aaxis. This magnetically-induced polarization ﬂop should be regarded as a magnetic
phase transition accompanied by the ferroelectric transition.
The zero-ﬁeld magnetic state below TC
was pinned down to a cycloid with thespin spiral plane perpendicular to the aaxis. The cycloid should induce electric polarization through the inverse effect of Dzyaloshinski-Moriya (DM) interaction. In contrast, the magnetic structure of the high-ﬁeld phase was not settled yet. From the theoretical point of view,
there are at least two possible spin arrangements which can induce electric polarization along the a axis. One is of the cycloid
type with the spiral plane perpendicular
to the c axis, and the other is of the commensurate collinear type with the propagation vector (0 1/4 1). A synchrotron x-ray
diffraction measurement in high magnetic
ﬁelds revealed that the propagation vector
changes from incommensurate (0 ≈ 0.27 1)
to commensurate (0 1/4 1). Judging fromthe phase diagram of the Gd1− x Tbx MnO3 ,the origin of the ferroelectric polarization
along the a axis should be common to thehigh-ﬁeld phase of TbMnO3 and the zeroﬁeld phase of Gd1− x Tbx MnO3 with x ∼0.3. As a full analysis of the magnetic structure in a high magnetic ﬁeld is not easy,
we investigated the magnetic structure of
Gd1− x Tbx MnO3 .
A single crystal of 160 Gd0.7 Tb0.3 MnO3
was grown by a ﬂoating zone method. Intensity data of magnetic reﬂections werecollected at 15 K by using a four-circle neutron diffractometer FONDER. The wavelength of 1.24Å was used for the measurement. The absorption of the neutron
beam by the crystal was 5.80/cm. Spin polarized neutron diffraction measurements
were performed with a triple-axis spectrometer PONTA. The intensity of a magnetic reﬂection (0 1/4 3) were investigated
for the incident neutron spin parallel andantiparallel to the scattering vector. In thisconﬁguration, the c component of the spin
vector chirality should cause a difference in
the intensity.
Figure 1 shows the proﬁles of magnetic
satellites at Qs = (0 1/4 3) for the ferroelectric state at 20 K after cooling in an electric ﬁeld. The intensity clearly depends on
the neutron spin direction. This result evidently indicates the chiral spin structure
in Gd0.7 Tb0.3 MnO3 . The magnetically induced polarization ﬂop in TbMnO3 is ascribed to the ﬂop of spiral plane around theb axis.

Fig. 1. Proﬁles of a magnetic reﬂection (0 1/4 3) in
160 Gd Tb MnO with the incident neutron spin
0.7
0.3
3
polarized (open red circles) parallel and (solid blue
circles) perpendicular to the scattering vector.

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1-3-27
Correlation between Electric Polarization and Sence of Helix in MnWO4
H. Sagayama(A), N. Abe(A), K. Taniguchi(A), T. Arima(A), M. Soda(B), M.
Matsuura(B), K. Hirota(B)(A)IMRAM, Tohoku Univ., (B)ISSP, Univ. TokyoInamagnetoelectriccompoundsinusoidal incommensurate
MnWO4 ,
antiferromagnetic ordering of the Mn2+
moments takes place at TN1 = 13.5 K witha magnetic wave vector with k ≈ (−0.214
1/2 0.457). The ferroelectric polarization
along the b axis (Pb ) emerges upon themagnetic phase transition from collinear tospiral spin structure at TN2 = TC = 12.7
K. Below TN3 = 7.6 K, the spin structure
alters into a commensurate collinear typewith k =(−1/4, 1/2, 1/2) and the ferroelectricn polarization is dismissed. We
report here the quantitative elucidation ofsuch magnetically induced ferroelectricity
in terms of the spin ellipticity as the orderparameter and show the successful electric
control between the clockwise (CW) andcounter-clockwise (CCW) spin helixes.
Spin-polarized neutron diffraction measurements were performed with a tripleaxis spectrometer PONTA at JRR-3. A single crystal was mounted on a sapphire
plate in a closed-cycle helium refrigerator
and irradiated with a spin-polarized neutron beam. A Heusler monochromator was
utilized to obtain the spin-polarized neutron beam. The spin of the neutron beam
could be ﬂipped by a spin-ﬂipper, so as tobe parallel or anti-parallel to the scatteringvector Qs with a guide-ﬁeld of about 10
gauss applied by a Helmholtz coil.
All the neutron diffraction measurements were performed in zero electric ﬁeld
after cooling the sample from the paramagnetic phase in a poling electric ﬁeld.
Peak proﬁles of magnetic satellite reﬂections with Qs =(−1 0 2)±k were measured
along the (−1 0 2) line in the reciprocal lattice.
Figure 1(a) shows the proﬁles of the magnetic satellites for the ferroelectric state at 9
K. The ﬂipping ratios are far from one only

for the ferroelectric phase (TN3 < T < TN2 ).
Moreover, the result shows that the senseof the spiral is controlled by the ferroelectric polarization direction. Such a behavior
seems to be common to the recently discovered magnetic ferroelectrics. However, theshort principal axis of the spiral of MnWO4
at 8K is estimated to be more than 90 % of
the long axis. This is rather a contrast to thecase of TbMnO3 , where the spiral is more
elliptic with mc /mb ∼ 0.7. The small ellipticity in this material is advantagious forthe investigation of low energy excitationsin the multiferroic.

Fig. 1. Proﬁles of magnetic satellites (−1 0 2 )±k inthree magnetic phases.

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JAEA-Review 2011-050

1-3-28Magnetic excitations of NaxCoO2.yD2O
Taketo Moyoshi, Yukio Yasui, Masatoshi Sato and Kazuhisa Kakurai1
Nagoya University, JAEA1
Na0.3CoO2.1.3H2O
withthe
2dimensional triangular lattice of Co atoms
exhibits the superconducting transition at
Tc of 4.5 K [1]. Because it attracted muchattention as the ﬁrst oxide superconductor
with 3d-electrons found after the high-Tc
Cu-oxides, various experimental and theoretical studies have been carried out toidentify the superconducting mechanism.
Here, we have carried out the neutron magnetic inelastic scattering to investigate therelationship between the magnetism andthe superconductivity. We used aligned
crystals of NaxCoO2.yD2O, in which thevolume fraction of the superconducting
phase (bilayer phase, y˜1.3) was about 75%
and the remaining non-superconducting
phase was found to be the non-deuterated
phase y˜0. Because parts of crystals exhibit
the superconducting transition at Tc˜ 4.5 K
and other parts exhibits the anomalies at
6 K by in the T dependences of the magnetic susceptibility and speciﬁc heat, we estimate the nuQ value of crystals to be ataround 12.5 MHz from the T-nuQ phase diagram reported in reference 2 (nuQ : 59Conuclear quadrupole frequency).
The neutron measurements were carriedout using the spectrometer 5G installed at
JRR-3 with the triple-axis condition. The
aligned crystals were used with the [100]and [001] axes in the scattering plane.
Constant-E scans along (h, 0, 2.8) have been
carried out at the energy transfer of 3 meVat several temperatures between 5 K and
100 K. In the measurement, the l value of
2.8 was chosen, because where the neutron
background count becomes almost minimum in the scan along (0, 0, l). Two magnetic scattering peaks have been observed
at h = 0 and h = 1/2. The peak at h = 0
is the two-dimensional ferromagnetic ﬂuctuation and expected to appear when theeg band pockets exist at the Fermi surface.

The spectral weight chi (Q, omega=3meV)at h = 0 decreases with decreasing temperature and disappears below 25 K. This result indicates that the two-dimensional ferromagnetic ﬂuctuation decreases with decreasing temperature and that the top of
the eg band is below the Fermi energy. In
contrast, the intensity at h = 1/2 seems toincrease slightly with decreasing temperature from 100 K to 5 K. Because the intensities of the magnetic excitations observed
at h = 0 at relatively high temperatures andh = 1/2 down to 5 K are almost constantwith varying l, the magnetic correlations
are two-dimensional character.
The present results exclude the possibilityof the triplet-pairing of the superconductivity, and are consistent with the resultsof the NMR Knight shift reported by thepresent authors group [3, 4].
Reference[1] K. Takada et al., Nature 422 (2003) 53[2] Y. Kobayashi, M. Yokoi, T. Moyoshi and
M. Sato, J. Phys. Soc. Jpn. 76 (2007) 103705.
[3] Y. Kobayashi, H. Watanabe, M. Yokoi, T.
Moyoshi, Y. Mori and M. Sato, J. Phys. Soc.
Jpn. 74 (2005) 1800.
[4] Y. Kobayashi, T. Moyoshi, H. Watanabe,
M. Yokoi and M. Sato, J. Phys. Soc. Jpn. 75(2006) 074717.

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1-3-29Magnetic structure of a pressure-induced magnetically ordered phase in YbAgGe
with a quasi-kagome lattice
K. Umeo(A), H. Kubo(B), T. Onimaru(B), K. Katoh(C), T. Matsumura(B), N. Aso(D) and
T. Takabatake(B)(A)N-BRAD, (B)ADSM, Hiroshima Univ., (C)NDA, (D)ISSP, Univ. Tokyo
The
heavy-fermion
antiferromagnet
YbAgGe with the ZrNiAl-type structure
undergoes two magnetic transitions at
TM1=0.8 K with an incommensurate
propagation vector k1=[0, 0, 0.324] andTM2=0.65 K with k2=[1/3, 0, 1/3] .[1,2] An
expanded tail in speciﬁc-heat C(T) above
TM1 is consistent with the magnetic frustration.[1] Recently, an anomalous phase
diagram of YbAgGe under pressures has
been constructed from the resistivity andC(T) measurements.[3,4] With applying
pressure above 0.5 GPa, the resistivity
anomalies at TM1 and TM2 merge into a
sharp drop at TM=0.85 K.[3] In the pressure
range 0.5 < P < 1.5 GPa, magnetic ordering temperature TM(P) remains constant,while above P* = 1.6 GPa, TM(P) increases
linearly. Concomitantly, the anomaly ofC(T) at TM converts from a ﬁrst-order typesharp peak to a second-order type jump ofa conventional magnetic compound without geometrical frustration. Additionally,
the magnetic entropy at TM rises for P> P*, while Kondo temperature does notchange.[4] These ﬁndings suggest that thesudden rise of TM(P) for P > P* is a dueto the release of the magnetic frustration.
In the present work, in order to determinea magnetic structure above 1.6 GPa, we
performed neutron diffraction experiments
under high pressure.
Measurements were preformed on a single
crystalline sample prepared by the Bridgman method. In neutron diffraction experiments, the sample was cooled down to 35
mK with a 3He-4He dilution refrigerator.
A pressure of 0.6 GPa was applying by apiston-cylinder cell (Cu-Be alloy, outer diameter=14mm) using Daphne oil as a pressure transmitting medium.
We found magnetic Bragg reﬂections at

Q=(1/3, 0, 1/3), (1/3, 0, 2/3), (2/3, 0, 1/3)and (2/3, 0, 2/3) at T=35 mK. Fig. 1 shows
the omega scan of the magnetic Bragg reﬂection at Q=(2/3, 0, 2/3) performed at
T=0.3 K and 1.13 K > TM. However, we observed no super lattice reﬂection with the
propagation vector k1=[0, 0, 0.324]. In order to investigate the magnetic structure
above 1.6 GPa, we are planning to performneutron diffraction measurements underhigher pressures.
[1] K. Umeo et al.: J. Phys. Soc. Jpn, 73(2004)537.
[2] B. Fak et al.: Physica B378-380 (2006)669.
[3] K. Umeo et al.: Physica B 359-361(2005)130.
[4] H. Kubo et al.: J. Phys. Soc. Jpn, 77 (2008)
in press.

Fig. 1. Omega scan of the magnetic Bragg reﬂection
at Q=(2/3, 0, 2/3). The closed and open circles correspond to the data at T=0.3 and 1.13 K, respectively.
The curves is a result of Gaussian ﬁtting.

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JAEA-Review 2011-050

1-3-30Spin excitations in MgCr2 O4
K. Tomiyasu1 , H. Suzuki2 , M. Toki3 , S. Itoh4 , N. Aso5 , M. Matsuura5 , K. Yamada1
WPI-AIMR Tohoku Univ.1 , Waseda Univ.2 , PF KEK3 , KENS KEK4 , ISSP Tokyo Univ.5
The geometric spin frustration is widely
accepted as a concept to bring out a novel
paramagnetic state. However, we measured two magnetic modes with discreteenergies in an antiferromagnetic orderedphase in a geometrically frustrated magnet MgCr2 O4 (spinel) by inelastic neutron
scattering on a single-crystal specimen, andclariﬁed the spatial spin correlations of thetwo levels: one is an antiferromagnetic hexamer and another is an antiferromagnetic
heptamer.
Figures 1(a) to 1(d) show the present neutron scattering data, the constant-E map
at E=4.5 and 9.0 meV in the hk0 and hhl
zones in the antiferromagnetic phase (T ∼5K). The data of (a) and (b) were measured
on HER, and those of (c) and (d) were
measured on PONTA and TOPAN, respectively. Figures 1(a) and 1(b) are the same
pattern as the quasielastic scattering in theparamagnetic phase, meaning the hexamer.
Figure 1(d) looks alike that of the independent seven-spin clusters (heptamers), proposed in the pyrochlore material Tb2 Ti2 O7
with the same magnetic lattice as the B sites
in a spinel material. We also conﬁrmed thatthe intensity pattern in another scattering
plane in Fig. 1(c) can be reproduced by theheptamer.
We now discuss the experimental factthat the one material includes the different
spatial correlations, which have been emblematic of the geometric spin frustrationin the paramagnetic phases of different systems. Also, such experiments will be able
to be expanded to the other frustrated magnets in the magnetic ordered phases.

Fig. 1. Color images of single-crystal inelastic scattering of MgCr2 O4 , measured in a constant energy
mode. The horizontal gauges indicate the scattering
intensity in arbitrary units.

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1-3-31

Magnetism and superconductivity in RENi2 B2 C

S. Ohira-Kawamura1 , R. Nagatomo2 , S. Konno3 , H. Kawano-Furukawa3 , H. Yoshizawa4
1 Academic and Information Board, Ochanomizu University
2 Department of Physics, Ochanomizu University
3 Graduate School of Humanities and Sciences, Ochanomizu University
4 ISSP-NSL, University of Tokyo
RENi2 B2 C (RE is a rare earth or Y)
has been studied intensively since a series of the materials exhibit various physical properties such as superconductivity,
magnetic order, or their microscopic coexistence with substituting the RE site. For
instance, one of them, ErNi2 B2 C, has attracted much attention because it exhibits
the coexistence of the superconductivity
and weak ferromagnetism. Recently, we
have made Lu0.5 Tb0.5 Ni2 B2 C as anotherpromising candidate in which the superconductivity and weak ferromagnetism coexist. In order to understand the magnetically ordered state in this system in detail,
we performed a neutron diffraction measurement.
Thesinglecrystalsampleof
Lu0.5 Tb0.5 Ni2 B2 C was prepared, andthe magnetic transitions at 9.5 K and 5.5 K
were conﬁrmed by a magnetization measurement. The sample was cooled down to
0.7 K using a 1K cryostat. The experiment
was carried out at the 4G spectrometer(GPTAS), and neutrons with a momentum
k i = 2.67 Å−1 were used. (h0l) was selected
as the scattering plane.
The neutron magnetic diffraction proﬁlesin the (h01) direction at 0.7 and 15 K areshown in Fig. 1(a). At 0.7 K, a clear magnetic Bragg peak is observed at Q = (0.44,0, 1), which corresponds to the propagation vector for the SDW state. In the caseof the pure TbNi2 B2 C system in the SDW
state, the higher-order peaks are also observed at the 3q, 5q and 7q positions in addition to q = 0.55a∗ . However, any othermagnetic peaks were not observed in thepresent study, indicating clear difference
from the pure system. The temperature dependence of the integrated intensity for the

Bragg peak at Q = (0.44, 0, 1) is displayedin Fig. 1(b). The SDW phase appears below ∼9.5 K. The q position of the observed
peak is not shifted with temperature. Moredetailed studies will be planned.

Fig. 1. (a) Neutron magnetic diffraction proﬁles inthe (h01) direction at 0.7 and 15 K. (b) Temperaturedependence of the integrated intensity of the magnetic Bragg peak at Q = (0.44, 0, 1).

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JAEA-Review 2011-050

1-3-32

Electronic state in novel superconductor CeCoIn5
studied by observation of the vortex state
H. Kawano-Furukawa1 , S. Ohira-Kawamura2 , S. Konno1 , R. Nagatomo3 ,H. Shishido4 , T. Shibauchi4 , Y. Matsuda4,5
1 Graduate School of Humanities and Sciences, Ochanomizu University
2 Academic and Information Board, Ochanomizu University
3 Department of Physics, Ochanomizu University
4 Department of Physics, Kyoto University
5 ISSP, University of Tokyo
CeCoIn5 is a new heavy fermion superconductor with quasi two-dimensional
electronic structure and the superconducting transition temperature Tc = 2.3 K. The
vortex state of this system has attracted agreat deal of attention, because some interesting phenomena have been reported. For
instance, a possible FFLO state has beensuggested in the low-T/high-H corner ofthe H-T phase diagram[1]. Recently we
performed a SANS experiment on this system in the perpendicular ﬁeld (H  c), andfound that the square ﬂux line lattice (FLL)
structure which was observed above 1 T exhibited reorganization to a triangular one
above 4 T and that the internal ﬁeld inside the vortex cores was unexpectedly enhanced by the external ﬁeld[2]. In order toinvestigate its FLL structure of CeCoIn5 in
H  a, we carried out a SANS experimenton this material.
The measurement was carried out at theC1-2 spectrometer (SANS-U). Neutrons
with wavelength of 7.08 Åwere used, and
the PSD was set at the 12 or 16 m position
from the sample. The single crystal samples (the average size of 3 × 0.5 × 0.5 mm3 )were aligned to cover the ∼ 8 × 8 mm2 area
so that the a axis is parallel to the neutron
beam and the c axis is parallel to the vertical direction. A 4 He cryostat with a 3 T
horizontal magnet was used, and the sample was cooled down to 1.6 K. The magnetic ﬁeld was applied parallel to the a axis
and the neutron beam.
The measurements were carried out at
0.1 T and 0.2 T. The data were collected at

1.6 K (T < Tc ), and the background datacollected at 3.5 K (T > Tc ) were subtracted.
We spent 6 hours to collect the data at eachtemperature. However, no reﬂections fromthe FLL were observed. The signal was notdetected even in the scattering vector (Q)dependence and the azimuthal angle (θ)
dependence of the scattering intensity. We
note that, in the case of the measurementfor H  c, the diffraction spots from the FLL
are clearly observed in shorter time.
The CeCoIn5 crystal has the tetragonal
symmetry (space group P4/mmm), and thesymmetry axis corresponds to the crystallographic c axis. When the magnetic ﬁeld
is applied parallel to the a axis (equivalent
for the b axis), the magnetic penetration
depths for the b and c directions, λ ab andλc , are expected to be signiﬁcantly different (λ ab is several times longer than λc ). In
this case, the supercurrent is expected to be
no longer circular but anisotropic. Namely,
the FLL structure should be distorted. On
the other hand, the sample angle ω was
calculated assuming isotropic triangular or
square FLL. Therefore, we currently expectthat the reason why the reﬂections were notobserved in the present study is that thechosen sample angle ω did not satisfy the
Bragg condition.
[1] See, for example, K. Kumagai et al.,Phys. Rev. Lett. 97 (2006) 277002.
[2] S. Ohira-Kawamura et al., J. Phys.
Soc. Jpn. (2008) in press.

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JAEA-Review 2011-050

1-3-33

Investigation of the magnetic excitations in high-TC
M. Matsuura1 , Y. Yoshida2 , H. Eisaki2 , N. Kaneko2 , and K. Hirota1
1 Institute for Solid State Physics, The University of Tokyo, 106-1 Shirakata, Tokai, 319-1106
2 AIST, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568

has been neglected in the study of magnetic
excitations in Bi2212.
References[1] H. F. Fong et al., Nature (London) 398, 588(1999).
[2] H. He et al., Phys. Rev. Lett. 86, 1610 (2001).
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( PH9䎗䎘䎘䎓F FRQVW(DW( PH9䎕䎙䎓䎓
&RXQWVPLQ

The interplay between antiferromagnetic(AF) spin ﬂuctuations and superconductivity is the central issue in the physics ofhigh-transition temperature superconductivity because of the persistent AF ﬂuctuations in the superconducting phase. Recently, a characteristic hourglass magnetic
excitation have been reported from two
families of high-Tc materials, LBCO andYBCO. If spin ﬂuctuations are important
for the mechanism of high-Tc superconductivity, they should be universal for all
copper-oxide systems, however, it is still
not clear. To resolve this issue, we exploredanother high-Tc system, optimmaly doped
Bi2.1 Sr1.9 CaCu2 O8+δ (Bi2212). Single crystals of Bi2212 were grown using travellingsolvent-ﬂoatingzone method.
Neutronscattering experiments were performed on
the triple-axis spectrometer PONTA installed at the JRR-3 Reactor of the JAEA. We
have aligned 9 single crystals on Al plates.
The total mass of aligned crystals is 6.4g
(0.98cc), which is 16 times as large as the
crystal used in the previous report[1].
Constant-Q spectrum taken in 2007 August show three peaks at 22, 36, and 46 meV(Fig.1a). We found 22- and 46 meV-peaks
are spurious peaks arising from incoherent
scattering of analyzer. Therefore, we improved 5G analyzer to reduce the incoherent scattering and the spurious peaks disapper for the 2007 Dec. spectrum (Fig.1a).
Thus, the scattering around 34 meV comesfrom sample, in addition, it increases below Tc as previous works.[1, 2] (Fig.1b)
Constant-E scan along the [110] direction at
E = 34 meV shows a peak at (π,π) whichis slightly enhanced below Tc (Fig.1c). One
shoud note that large peak at (π,π) andE = 34 meV remains even at T = 100 K(> Tc ). This suggests that strong spin ﬂuctuations exist in the normal state, which7 .
.

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Fig. 1. Const-Q spectra at (1/2 1/2 -14) and T =1.2 K (T < Tc ) and 100 K (T > Tc ). b) ConstantEnergy proﬁles at h̄ω = 34 meV with (hh-14).

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-3-34Magnetic Structure in the Shastry-Sutherland Lattice Tb1-xYxB4
F. Iga(a), S. Michimura(a), K. Murakami(a), T. Takabatake(a), K. Suga(b), K. Kindo(b), K.
Ohoyama(c)(a)ADSM, Hiroshima Univ., (b) ISSP, Univ. of Tokyo, (c) IMR, Tohoku University
Rare-earth tetraborides RB4 have a tetragonal crystal structure with a space group
P4/mbm which is characterized by the 2dimensional orthogonal dimers in the cplane. Such dimer systems are equivalent to the Shastry-Sutherland lattice (SSL)
where nearest-neighboring dimers havegeometrical frustration.
TbB4 has successive antiferromagnetictransitions at TN1 = 44 K and TN2 = 24 K.
The magnetization curve of TbB4 at 1.3K
shows at least nine magnetization jumps
above 16T for B//c and it is remarkableconcerning the origin. In order to approach
the mechanism of multi-step magnetization, we studied Y-substitution effect on
TbB4 for magnetic susceptibility, magnetoresistance and speciﬁc heat. From thesemacroscopic measurements the characteristic temperature TN2 was found to besmeared out around x=0.2.
In order to clarify whether such lower
temperature phase below TN2 truly disappears at x=0.2 or not, we have measured
the powder neutron diffraction for x=0.10
and 0.25. The isotope boron 11 enriched up
to 99.75% was used for sample preparationand these samples were crushed to powder. The neutron powder diffraction experiment was performed by using HERMES.
Measured temperature region were from 3
to 50 K. For x=0.1 this alloy shows successive antiferromagnetic phase transition at
TN1 = 40 K and TN2 = 20 K. Below TN1,
magnetic peaks at (100), (210) and (111)
gradually grow with decreasing temperature. Furthermore these magnetic peaks
grow again below TN2 = 20 K. On the other
hand, magnetic peaks for x=0.25 graduallygrow below TN1 = 35 K and these intensities saturate at 20 K. From these measurement, we could not ﬁnd another phasetransition correspondent to TN2 for x=0.25.

Fig. 1. Temperature dependences of some magnetic
peaks at (110), (111) and (210) in x=0.10 and 0.25.

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JAEA-Review 2011-050

1-3-35

1st order transition in ErNi2 B2 C

H. Kawano-Furukawa, Y. Ishida , S. Ohira-Kawamura, H. Yoshizawaa and H. Takeyab
Ochanomizu Univ., ISSP NSL Univ. of Tokyoa and NIMSb
ErNi2 B2 C is the ﬁrst material in which
a microscopic coexistence of weak ferromagnetism (WFM) and superconductivity(SC) was directly conﬁrmed by a neutron
scattering measurements in zero ﬁeld [1].
ErNi2 B2 C transforms to a superconducting
state at Tc = 10.5 K, a SDW state at TN = 6K
and a weak ferromagnetic state at TWFM =2.3K. At early stage of the study, Zarestky
et. al. [2] and Sinha et. al. [3] independently performed neutron diffraction measurements and both group independently
observed that clear magnetic peaks develope below TN at incommensurate wave
vector q ∼ 0.553a* and spins on Er atoms
order transversely polarized planar sinusoidal structure. After these works, we performed unpolarized and polarized neutron
diffraction measurements and succeededin conﬁrming microscopic coexistence between the WFM and the SC by showing
an appearance of an interferance term below ∼ 2.3K at both (0 0 2) and (0 0 6) nuclear Bragg positions of the ErNi2 B2 C crystal [1,4]. In those studies, however, we noticed that temperature dependence of themagnetic intensity shows a hysteresis behavior around 2.3K. To check an origin of
this anomaly, we performed further neutron diffraction measuremtns.
In the present study, we used single crystals of ErNi11
2 B2 C grown by a ﬂoating zone
method. Tc of our un-annealed sample isdetermined to be ∼ 8.6 K which is same
crystal with the one used in the previous
experiment [1].
Figures show temperature dependenceof neutron diffraction intensities at (a)(1 0 0) and (2) (0 0 1). These two points areequivalent Bragg positions for the WFM
order parameter. But data show different
temperature dependence around 2.3K. This
result indicates a rotation of spins. To checkthis behavior in more detail we measured

neutron diffraction proﬁles along (h 0 1)
and (h 0 0) (not shown). With such date,
we concluded that that the ferromagnetic
order in ErNi2 B2 C ﬁrst develops with spins
along the a-axis below 2.3K but it rotate
along the b-axis at 1.8K through a ﬁrst order transition.
[1] H. Kawano et al., J. Phys. Chem.
Solids 60, 1053 (1999)[2] J. Zarestky et al., Phys. Rev. B 51, R678
(1995).
[3] S.K. Sinha et al., Phys. Rev. B 51, R681
(1995).
[4] H. Kawano-Furukawa et al., Phys.
Rev. B 65, 180508 (2002)

Fig. 1. Temperature dependence of Bragg intensities
at (a) (1 0 0) and (b) (0 0 1).

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-3-36

Study of spin ﬂuctuations in La1.94−x Srx Ce0.06 CuO4

M. Fujita1 , M. Enoki2 , and K. Yamada3
1 Institute for Materials Research, Tohoku University, Katahira, Sendai 980-8577, Japan
2 Department of Physics, Tohoku University, Aramaki, Sendai 980-8578, Japan
3 World-Premier-International Research Center Initiative,
Tohoku University, Katahira, Sendai 980-8577, Japancurs in the system with corrugated CuO2
planes. Moreover, the appearance of gaplike structure in χ (ω) by reducing the lattice distortion would be the evidence forthe existence of spin-gap states in the underdoped La214 system. Further systematic neutron-scattering experiments are required to clarify the intrinsic spin correlations in the high-Tc superconductors.
References[1] M. A. Kastner et al.: Rev. Mod. Phys. 70,(1998)897.
[2] M. Fujita et al.: Phys. Rev. Lett. 88(2002)167008.
[3] C.H. Lee et al.: J. Phys. Soc. Jpn. 69(2000)1170.
La1.94-xSrxCe0.06CuO4, T 8K
1.5(a) x=0.14

1.0

TOPAN
HER

0.5

χ" (arb. unit)

It is widely believed that spin correlations play an important role in themechanism of high-Tc superconductivity[1]. Since, the static spin order competes
with the superconductivity and such orderis stabilized in the system with corrugated
CuO2 planes[2], a study of spin ﬂuctuations in the system with ﬂat CuO2 plane,
where the ideal superconducting state isconsidered to be realized, is more important. In order to shed light on this issue,
we have carried out neutron-scattering experiments to investigate the effect of distortion of CuO2 planes on the low-energy spincorrelation of La1.94− x Srx Ce0.06 CuO4 with
x=0.14, 0.18 and 0.24, of which orthorhombic lattice distortion is smaller than thatin La2− x Srx CuO4 (LSCO) with comparable hole concentration.
As shown in Fig. 1, clear gap structure
was observed in the energy spectrum of local dynamical susceptibility χ (ω) for bothx=0.18 (p∼0.14) and x=0.24 (p∼0.20) samples, similar to the results for optimallydoped LSCO[3]. On the other hand, in the
x=0.14 (p∼0.10) sample, a low energy component showing the increases of intensity
below 2∼3meV with lowering ω was observed within the gap-like structure. Sucha χ (ω) in x=0.14 is quite different fromthat for LSCO with x  =0.10, although theeffective hole concentration in two samples
is comparable[3]. These experimental results suggest that the gap-strucure is robust
against the lattice distortion, while the loweneryg component is strongly inﬂuenced
by the lattice distortion. We speculate thatsuch reduction of the low-energy component is caused by the relaxation of corrugation of CuO2 planes. In other words,
the slowing down of spin ﬂuctuations oc-0(b) x=0.18

1.0
0.5
0

(c) x=0.24

1.0
0.5
0

0

5

10

15

Energy (meV)
Fig. 1.
Local spin susceptibility forLa1.94− x Srx Ce0.06 CuO4 with (a) x=0.14, (b) 0.18 and(b) 0.24 measured below 8 K.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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1-3-37

Search for transition of paring symmetry in electron-doped superconductor
Pr1−x LaCex CeO4
M. Fujita1 , M. Nakagawa2 , and K. Yamada3
1 Institute for Materials Research, Tohoku University, Katahira, Sendai 980-8577, Japan
2 Department of Physics, Tohoku University, Aramaki, Sendai 980-8578, Japan
3 World-Premier-International Research Center Initiative,

Tohoku University, Katahira, Sendai 980-8577, Japan
shown. Intensity of phonon gradually increases upon heating. The increase of intensity can be reproduced by thermal factor and no clear anomalous temperaturedependence of phonon was observed inthis sample within the experimental accuracy. However, to conclude the absenceof anomaly in phonon, more precise measurement with high energy resolution is required and comprehensive study for wide
concentration range is important for the
next step.
References[1] M. Tachiki et al.: Phys. Rev. B 67 (2003)174506.
[2] S. Ishihara and N. Nagaosa: Phys. Rev. B 69
(2004)144520.
Phys. Rev. Lett 88(2002)207005.
[4] V.A. Khodel et al.: Phys. Rev. B 69 (2004)144501.

[3] J.A. Skinta et al.:Pr0.85LaCe0.15CuO4

20
15

Q=(0.1, 0, 4)

T=8K

10
5
0
15

T=12K

10

Counts/min

Research of mechanism of high-Tc superconductivity remains one of central issues in the strongly correlated electron system. Extensive research on the magnetismin the cuprate superconductors revealed
the close relation between the spin correlations and the hihg-Tc superconductivity. On the other hand, a possible role oflattice vibrations in the mechanism of thehigh Tc superconductivity has also been intensely studied[1,2]. Quite recently, an evidence for the transition or crossover of superconducting paring symmetry from being d-wave to s-wave in nature upon doping was reported for the electron-doped (ntype) cuprate[3,4]. This suggests that in
the n-type superconductors the d-wave superconductivity mediated by spin ﬂuctuations can change to the conventional swave superconductivity mediated by lattice vibrations with increasing doping concentration. In comparison, such symmetry crossover has not been reported in thecase of the p-type cuprates, suggesting thatthe d x 2 -y 2 -wave symmetry favoring a spinmediated mechanism seems to be common in the whole range of p-type high-Tc
cuprates. Therefore, to understand common mechanism of high-Tc superdonductivity, it is quite important to clarify theorigin of s-wave superconductivity in theelectron-doped system.
Motivated by above reason, we havestarted the neutron-scattering study on the
n-type Pr1− x LaCex CuO4 system to conﬁrm
the evidence of s-wave superconductivity.
In Fig. 1, preliminary results for the measurement of an acoustic phonon around (00 4) position in x=0.15 sample (Tc =16 K) are

5
0
15

T=15K

10
5
0

T=25K

15
10
5
0

0

1

2

ω (meV)

3

4

Fig. 1. Constant-momentum spectra with Q=(0.1, 0,4) in Pr0.93 LaCe0.07 CuO4 measured at temperatures
around Tc (=16 K).

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-3-38Zn-doping eﬀect on spin ﬂuctuations in electron-doped Pr1−x LaCex CuO4
M. Fujita1 , M. Nakagawa2 , and K. Yamada3
1 Institute for Materials Research, Tohoku University, Katahira, Sendai 980-8577, Japan
2 Department of Physics, Tohoku University, Aramaki, Sendai 980-8578, Japan
3 World-Premier-International Research Center Initiative,
Tohoku University, Katahira, Sendai 980-8577, Japanthe similarity suggest that the doped electrons dilute Cu spins on CuO2 planes.
References[1] K. Yamada et al.: Phys. Rev. Lett 90(2003)137004.
[2] M. Fujita et al.: arXiv:0707.0150.

Count/5.4min

400Count/4.2min

Pr0.89LaCe0.11Cu0.986Zn0.014O4, T=4K

400

(a)

(h 0 0)ω=4meV200

0ω=7meV
200

Count/8.9min

0ω=10meV

600
400
200
0
0.8

0.9

1.0

1.1

1.2

h (r.l.u.)
0.08

Pr0.89LaCe0.11Cu1-yZnyO4, T<8K
peak-width(r.l.u.)

In the hole-doped (p-type) high-Tc
cuprates, extensive neutron-scattering
measurement clariﬁed that antiferromagnetic spin ﬂuctuations in doped Mott
insulators show close connection withhigh-Tc superconductivity. However, lessis known about the spin correlations in theelectron-doped (n-type) supercondcuting
cuprates. Neutron-scattering experimenton n-type Nd2− x Cex CuO4 revealed the existence of commensurate low-energy spincorrelations in both AF ordered and SC
phases [1]. This is qualitatively different
from the well-deﬁned incommensurate
structure observed in the p-type cuprates,
and it implies that the microscopic originof the superconductivity in cuprates might
be asymmetric against the type of charge
carriers. To clarify the nature of spincorrelations in the electron-doped systemthrough impurity effect, we performed inelastic neutron-scattering measurement on
Pr0.89 LaCe0.11 Cu1−y Zny O4 with y=0.014.
Fig. 1 shows constant-q spectra measured at 3 meV, 7 meV and 10 meV. Welldeﬁned commensurate peak was observedat all energies, analogous to the results for
Zn-free Pr0.89 LaCe0.11 CuO4 . However, thepeak is somewhat broader than that in Znfree sample. In Fig. 2, peak-width (halfwidth at half-maximum) as a function ofω obtained by ﬁtting to a single Gaussian
without convoluting the instrumental resolution is shown. The results for Zn-freesample is also plotted as a reference. In
both samples, the width increases linearlywith increases ω. However, the slope, κ/ω,is larger in the Zn-doped sample. Such a
increase of slope by Zn-doping is similar to
the result for the evolution of spin correlations by electron-doping[2], and therefore

0.06

(b)

0.04

y=0
y=0.014

0.0
2
0

0

5

10

15

ω (meV)
Fig. 1.
(a) Constant energy spectra for
Pr0.89 LaCe0.11 Cu0.986 Zn0.014 O4 . (b) ω-dependenceof peak-width for Zn-free and Zn-doped samples.

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JAEA-Review 2011-050

1-3-39Order Parameter of Phase IV in (Ce,La)B6

K. Kuwahara, K. Iwasa(A), M. Kohgi, N. Aso(B), M. Sera(C), F. Iga(C), M. Matsuura(B),K. Hirota(B)Department of Physics, Tokyo Metropolitan University, Department of Physics Tohoku
University(A), Neutron Science Laboratory, Institute for Solid State Physics, University ofTokyo(B), Department of Quantum Matter, ADSM, Hiroshima University(C)Recently we have observed weak but
distinct superlattice reﬂections at Q =(h/2,h/2,l/2) (h, l = odd number) fromphase IV of Ce0.7La0.3B6 for the ﬁrst timeby elastic neutron scattering. The intensityof the superlattice reﬂections is stronger
for high scattering vectors. This unusual
Q dependence of the intensity evidencesthat the order parameter of phase IV has acomplex magnetization density, consistent
with the recent experimental and theoretical prediction in which the order parameter is the magnetic octupoles T beta withGamma 5 symmetry of Oh. However, it
still remained possible that such a Q dependence of intensity might arise from lattice
distortions, since the scattering intensity
due to lattice distortions also increases withincreasing Q in proportion to the square of
Q. To rule out this possibility, we have performed further neutron scattering experiments.

(5G). Spin-ﬂip neutron scattering havebeen clearly observed. This provides direct
evidence that the observed superlattice reﬂections are magnetic and not due to lattice
distortions.

CountsCerium hexaboride CeB6 undergoes successive phase transitions from paramagnetic phase (Phase I) to antiferroquadrupolar ordering and to antiferromagnetic ordering (Phase III). By doping La into theCe site in this system, a new phase calledphase IV appears in CexLa1-xB6 for x < 0.8.

Fig. 1. Neutron scattering patterns of rocking curves
at the scattering vector Q = (5/2,5/2,5/2), where thespin of the incident neutrons is parallel (the spin
ﬂipper was off) or antiparallel (the spin ﬂipper wason) to the scattering vector Q.

A large single crystal of Ce0.7La0.3B6 wasgrown by the ﬂoating zone method, using
99.52% enriched 11B to avoid the large neutron absorption due to 10B. The neutron
diffraction experiments were performed on
the thermal neutron triple axis spectrometer TOPAN (6G) & PONTA (5G).
Figure 1 shows the result of the polarized
neutron scattering experiment at PONTA
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JAEA-Review 2011-050

1-3-40

Neutron scattering study on PrFe4P12 under high pressure

K. Kuwahara, T. Osakabe(A), K. Iwasa(B), M. Kohgi, D. Kikuchi, Y. Aoki, H. Sato, H.
Sugawara(C)Department of Physics, Tokyo Metropolitan University, Neutron Materials Research Center,
Japan Atomic Energy Agency(A), Department of Physics, Tohoku University(B), Faculty ofIntegrated Arts and Sciences, The University of Tokushima(C)In order to get further microscopic information about the pressure-induced antiferromagnetic order, we have performed highpressure neutron diffraction measurements
on PrFe4P12 single crystal at low temperatures under high pressure and magnetic ﬁelds using the triple-axis spectrometer TOPAN at JRR-3M in JAEA and the
HAC. Single crystals were grown by tinﬂux method. The HAC was set inside a superconducting magnet with the [0,0,1]-axis
vertical to the (h,k,0) scattering plane.

perzone gap formation at the Fermi surface
due to the antiferromagnetic order, since
the Fermi surface of an extra hole-like band
exists. Further studies are necessary to clarify the mechanism of the M-I transition.
14.77Ei, Open-PGf-BG-BG-BG, 3axis

14.77Ei, Open-PGf-BG-BG-BG, 3axis
6000

6000

PrFe4P12

P=3.2GPa
B=0T

5000

(1,0,0)
4000

T_dec
3000

2000
0

Counts/12min(6645Kmon)

PrFe4P12Counts/12min (6645Kmon)

PrFe4P12 undergoes the non-magnetic
phase transition at TA = 6.5 K under ambient pressure. By applying pressure, thenon-magnetic ordered phase disappears
and the metal-insulator (M-I) transition occurs around Pc = 2.4 GPa (Hidaka et al.:Phys. Rev. B 71 (2005) 073102). In theinsulating phase, we have observed thedistinct antiferromagnetic magnetic Bragg
peak with a wave vector q =(1,0,0) above
Pc by using a new hybrid-type pressure cell(HAC) which is composed of a large sapphire anvil and a tungsten carbide anvil(Osakabe et al.: J. Mag. Mag. Mat. 310(2007) 2725).

P=3.2GPa
T=1.7K

5000(1,0,0)
4000

3000

2000
5

10

15

Temperature (K)

20

0

1

2

3

4

5

6

B (T)

Fig. 1. Temperature and magnetic ﬁeld dependences of the antiferromagnetic Bragg peak with q= (1,0,0) under 3.2 GPa.

Figure 1 shows the temperature and magnetic ﬁeld dependences of the antiferromagnetic Bragg peak with q = (1,0,0) under 3.2 GPa. The pressure-induced antiferromagnetic order is clearly suppressed byapplying magnetic ﬁeld. This result agrees
with the reported ﬁeld dependence of theelectrical resistivity. This strongly indicatesthat the pressure-induced M-I transitionis caused by the antiferromagnetic order.
However, it is difﬁcult to explain the mechanism of the M-I transition by a simple suActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-3-41

Rattling motion in PrOs4Sb12

K. Kuwahara, O. Yamamuro(A), K. Iwasa(B), M. Kohgi, D. Kikuchi, Y. Aoki, H. Sato, H.
Sugawara(C)Department of Physics, Tokyo Metropolitan University, Neutron Science Laboratory, Institutefor Solid State Physics, University of Tokyo(A), Department of Physics, Tohoku University(B),Faculty of Integrated Arts and Sciences, The University of Tokushima(C)below around 0.2 meV. The observed excitation might be due to the rattling motion of Pr-ion. To clarify this possibility, further studies, such as measurements of Qdependence of the excitation, are needed.

0.15
100K
10K

0.10

S(Q,w)

The ﬁlled skutterudite compounds RT4X12(R: rare earth or actinide, T: transition
metal, X: pnictogen) crystallize in thebody-centered cubic space group Im-3,
in which R ion is surrounded by acage of X-icosahedron. This characteristic ”cage” structure provides a wide variety of thermal, magnetic and transport
properties. Among the ﬁlled skutterudite
compounds, PrOs4Sb12 received much attention because it is the ﬁrst Pr-based
heavy-fermion superconductor and a ﬁeldinduced antiferro-quadrupolar (AFQ) ordered phase exists near the superconducting phase. In addition to the relation between the AFQ ﬂuctuations and the superconductivity, interestingly, the possibility that the heavy-fermion superconductivity is related to a rattling motion due
to a weakly bounded Pr-ion in the Sb
cage has been argued. Especially, a Debyetype dispersion in the elastic constants observed by high resolution ultrasonic measurements (T. Goto et al.: Phys. Rev. B 69
(2004) 180511R) shows the importance ofthe rattling motion in this system. In order to microscopically study the dynamical
property of the rattling motion, we started
doing inelastic neutorn scattering experiments with high energy resolution.

0.05

0.00
-1.0

-0.5

0.0

0.5

1.0

E (meV)

Fig. 1. Inelastic spectra of PrOs4Sb12 at 10 K and
100 K.

The powder sample of PrOs4Sb12 wasgrown by Sb-self-ﬂux method. The total
mass is about 39 g. The inelastic neutorn
scattering experiments were done by using the Angle Focusing Cold Neutron Spectrometer (AGNES) at JRR-3M in JAEA.
Figure 1 shows inelastic spectra at 10 K and
100 K. The difference between spectrum at
10 K and that at 100 K has been observed
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1.  ਛᕈሶᢔੂ 4 㕖᥏⾰㨯ᶧ૕ 


1. Neutron Scattering

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JAEA-Review 2011-050

1-4-1
Direct observation of supercooled water in hardened Low Heat Portland Cement
K. Mori(A), Y. Inamura(B), O. Yamamuro(B), T. Fukunaga(A)(A)Research Reactor Institute, Kyoto University, (B)ISSP, University of Tokyo
Frost damage on concrete buildings is oneof the most serious problems in cold districts like Hokkaido in Japan. Freezing ofwater makes its own volume increase up
to as much as 9%, inducing internal pressure within concrete materials. However,the freezing and thawing cycle of water isvery complicated due to an existence of supercooled water below 273 K. In this work,
we performed directly to observe the freezing and thawing water in hardened Low
Heat Portland Cement (LHPC) by using
the quasi-elastic neutron scattering (QENS)
method.
The LHPC clinkers were hydrated withlight water (H2O) at 301 K in air. The H2O
to LHPC mass ratio is 0.5. After a coupleof days, the hardened LHPC was soaked inwater. QENS data of the hardened LHPC
were measured at temperatures between
202 K and 302 K on the high-resolution
pulsed cold neutron spectrometer, AGNES,
installed at the ISSP at University of Tokyo.
The energy resolution of the AGNES is 120
μ eV when the neutron wavelength is 4.22
angstrom.
Figure 1 (a), (b), (c) and (d) show QENS
spectra at 302 K, 272 K, 262 K and 242
K. The closed and opened circles indicate
the freezing and thawing processes, respectively. The solid line is the QENS spectrum
at 202 K, corresponding to the energy resolution of the AGNES. This means thatthe water in the hardened LHPC freezes
completely below 202 K. Above 242 K, the
QENS was clearly observed, that is, the supercooled water exists at temperatures between 242 K and 273 K. Furthermore, it
was found that the freezing and thawing
cycle of water in the hardened LHPC has
a little hysteresis below 273 K.
Fig. 1. QENS spectra at 302 K, 272 K, 262 K and 242
K.

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1-4-2
Neutron Diﬀraction Study on the Intermolecular Structure in Highly Concentrated
Aqueous Urea Solutions
Yasuo Kameda, Asami Maki, Hiroaki Takahashi, Yuko Amo, Takeshi Usuki
Department of Material and Biological Chemistry, Faculty of Science, Yamagata University,
Yamagata 990-8560
Intermolecular hydrogen-bonded structure in the concentrated aqueous urea solution has been received much attention because of its importance for various ﬁelds ofchemical and biological sciences. A number of neutron diffraction studies have been
conducted in order to investigate the hydration structure of the urea molecule [1-6],
however, direct experimental informationon the structure of urea-urea interaction
has not yet been obtained. In the present
report, we describe results of neutron
diffraction measurements on 14N/15N and
H/D isotopically substituted aqueous 25
mol% urea solutions in order to obtainthe N(urea)-N(urea) partial structure factor and corresponding N-N partial distribution function.
Five isotopically substituted aqueous 25
mol% urea solutions were used in thepresent study, namely,
I. [(14ND2)2C=O]0.25(D2O)0.75,
II. [(15ND2)2C=O]0.25(D2O)0.75,
III. [(14-15ND2)2C=O]0.25(D2O)0.75,
IV. [(14NZ2)2C=O]0.25(Z2O)0.75, andV. [(15NZ2)2C=O]0.25(Z2O)0.75,
where 14-15N is the 1:1 mixture of 14N and
15N, and Z denotes the null mixture of
H and D. Sample solutions were sealed ina cylindrical quartz cell (12.0 mm in innerdiameter and 1.1 mm in thickness).
Neutron diffraction measurements werecarried out at 298 K using the ISSP diffractometer 4G (GPTAS) installed at the JRR3M research reactor with an incident neutron wavelength of 1.099(4) A. Scatteredneutrons were collected over the angularrange of 3 < 2 theta < 118 deg. corresponding to 0.30 < Q < 9.80 1/A. Preset timewas 230 s for each data point. Measure-ments were made in advance for an empty
cell, a vanadium rod of 10 mm in diameter, and an instrumental background. After correction for the background, absorption and multiple scattering, the observedcount rates were converted to the scatteringcross section by the use of corrected scattering intensities from the vanadium rod.
The intermolecular ﬁrst-order differencefunction, delta-N-inter(Q) [7], was derived
from the difference in observed scatteringcross sections between sample solutions
that have different average coherent scattering length of the nitrogen atom. The
observed delta-N(Q) function can be described by a linear combination of the partial structure factors involving contribution
from the nitrogen atom. Numerical valuesof the coefﬁcients A - D are summarized inTable 1.
delta-N(Q) = A[aNO(Q)-1] + B[aNH(Q)-1]+ C[aNC(Q)-1] + D[aNN(Q)-1],
where,
A = 4x delta bN bO,
B = 8x(1+x) delta bN bH,
C = 4x**2 delta bN bC, andD = 4x**2(bN**2 - bN **2).
Table 1. Weighting factor for partial structure factors in the ﬁrst- and second-orderdifference functions (in barns).
——————————————————Difference
A
B
C
D——————————————————I - III
0.0830 0.2383 0.0238 0.0618
III - II
0.0830 0.2383 0.0238 0.0516(I-III)-(III-II) 0000.0102——————————————————-

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JAEA-Review 2011-050

The N-N partial structure factor was successfully obtained from the second-orderdifference between two ﬁrst-order difference functions, between samples I - III and
III - II. Although observed intermolecular difference functions between samples I- III and III - II look very similar, the derived N-N partial structure factor clearly
indicates the ﬁrst diffraction peal at Q =1.5 1/A. Difference distribution functions
GN(r) between samples I - III and III - II,and the N-N partial distribution function
are represented in Fig. 1. The observed intermolecular N-N partial distribution function, gNN(r), is characterized by a wellresolved ﬁrst peak at r = 5 A, which may
imply that that the stable urea cluster ispresent in the concentrated aqueous solution. Detailed structural information on
the N-H and N-O partial structure functions can be obtained from the combinationof the observed scattering cross sections forsamples I - II and IV - V, respectively. Further data analysis is in progress.
References[1] J. L. Finney, J. Turner, Ann. N.Y. Acad.
Sci., 482 (1986) 127.
[2] J. L. Finney, J. Turner, Electrochim. Acta,
33 (1988) 1183.
[3] J. L. Finney, A. K. Soper, Chem. Soc.
Rev., 23 (1994) 1.
[4] Y. Kameda, H. Naganuma, K.
Mochiduki, M. Imano, T. Usuki, O.
Uemura, Bull. Chem. Soc. Jpn., 75 (2002)
2579.
[5] A. K. Soper, E. W. Castner, A. Luzar, Biophys. Chem., 105 (2003) 649.
[6] Y. Kameda, M. Sasaki, S. Hino, Y. Amo,
T. Usuki, Bull. Chem. Soc. Jpn., 79 (2006)
1367.
[7] J. E. Enderby, G. W. Neilson, Water,
A Comprehensive Treatise , Plenum Press,
New York, (1979), Vol. 6, p. 1.

Fig. 1. a, b) Intermolecular difference distributionfunctions and c) N-N partial distribution function
observed for aqueous 25 mol% urea solutions.

1-4-2

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JAEA-Review 2011-050

1-4-3
SANS Study on Mixing State of Ionic Liquid-Molecular Liquid Binary Solutions
Toshiyuki Takamuku, Yusuke Honda, and Kenta Fujii
Saga University
Recently, ionic liquids and their mixturesof molecular liquids are frequently examined as a novel solvent for electric devices,
organic syntheses, and solvent extractions.
However, physicochemical properties ofionic liquids and ionic liquid-molecularliquid mixtures are still unknown at themolecular level. The properties are essential to understand chemical reactions andequilibria in ionic liquids and their mixtures of molecular liquids.
In the present study, mixing state of binary solutions of imidazolium-based ionicliquids and water, methanol, acetonitrile,and benzene has been observed at a mesoscopic level by using small-angle neutron
scattering (SANS) technique. Two ionic liquids, 1-ethyl-3-methylimidazolium (EMI+)
chloride (Cl-) (m.p. = 360 K) and EMI+ bis(triﬂuoromethanesulfonyl) amide (TFSA-)(m.p. = 256 K) were examined. Based on thepresent results, the effects of the propertiesof the molecular liquids on mixing state ofionic liquid-molecular liquid binary solutions have been discussed.
Sample solutions were prepared bydissolving EMICl into deuterated liquids of water, methanol, and acetonitrile
and by mixing EMITFSA with deuterated methanol, acetonitrile, and benzene atvarious mole fractions. However, EMIClbenzene and EMITFSA-water solutions
were not prepared because of their very
low miscibility. SANS spectra of the sample solutions at 298 K were measured on
the SANS-U spectrometer with the camera
lengths of 1 and 4 m. The scattering intensities for the sample solutions were accumulated on the detector at the camera lengthsof 1 and 4 m for 10 min and 1 h, respectively.
For the EMICl systems, as seen in Fig.
1(a), the SANS intensities for the EMIClacetonitrile mixtures are signiﬁcantly ob-

served at the high acetonitrile mole fractions of 0.8, 0.9, and 0.95. However, theSANS intensities for the EMICl-water and
EMICl-methanol mixtures were scarcely
observed. Thus, EMICl and acetonitrile
molecules form each cluster in the mixtures, whereas EMICl is homogeneously
dissolved into water and methanol. On
the other hand, for the EMITFSA systems,
the SANS intensities for the EMITFSAmethanol mixtures are signiﬁcant at themethanol mole fractions of 0.8, 0.9, and0.95 as shown in Fig. 1(b), while those for
the EMITFSA-acetonitrile and EMITFSAbenzene mixtures were not observed.
Hence, both EMITFSA and methanol are
inhomogeneously mixed each other in the
mixtures, but acetonitrile and benzene arehomogeneously mixed with EMITFSA.
The present results can be explained asfollows. In the EMICl systems, acetonitrile
molecules may not strongly interact with
Cl- due to the low electron-acceptabilityof acetonitrile, while water and methanol
molecules strongly solvate Cl-. However,benzene molecules cannot solvate highly
charged Cl- i.e., EMICl is not dissolved
into benzene. These are the reasons for themost inhomogeneous mixing of the EMIClacetonitrile mixtures among the EMICl systems. On the contrary, methanol molecules
weakly interact with TFSA- because of the
low charge-density of TFSA-. However,acetonitrile molecules can easily interact
with TFSA- due to the suitable polarity ofacetonitrile. In contrast, water molecules
hardly interact with hydrophobic TFSA, i.e., a small amount of water is only
dissolved in EMITFSA. In the EMITFSAbenzene mixtures, benzene molecule may
contact with EMI+ by the pi-pi interaction between them [1,2]. Additionally, benzene molecule may easily interact with
low-charged TFSA-. It results in the homo-

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JAEA-Review 2011-050

geneous mixing of the EMITFSA-benzene
mixtures. Thus, the inhomogeneity of the
EMITFSA-methanol is the highest among
the EMITFSA systems.
[1] C.G. Hanke, A. Johansson, J.B. Harper,
and R.M. Lynden-Bell, Chemical Physics
Letters 374, 85-90 (2003).
[2] M. Deetlefs, C. Hardacre, M. Nieuwenhuyzen, O. Sheppard, and A. K. Soper, J.
Phys. Chem. B, 109, 1593-1598 (2005).

Fig. 1. SANS spectra for (a) EMICl-acetonitrile and(b) EMITFSA-methanol mixtures.

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JAEA-Review 2011-050

1-4-4

Amide-Induced Phase Separation of HFIP-Water Mixtures
Toshiyuki Takamuku, Hiroshi Wada, and Kenta Fujii
Saga University
Aqueous mixtures of several watermiscible organic solvents, such as propanol
and acetonitrile, separate into organic
solvent-rich and water-rich phases, whensalt is added into mixtures. The key ofthe salt-induced phase separation is preferential solvation of both cation and anion by water molecules [1-4]. Thus, water
clusters are evolved around both ions withincreasing salt concentration, and organic
molecules, which are excluded from water
clusters, simultaneously aggregate to form
clusters. Finally, phase separation takes
place, when the size of both water clusters and organic solvent clusters reaches amacroscopic scale. Recently, we have foundthat addition of amphiphilic molecules,
such as amide, also induces phase separation of 1,1,1,3,3,3-hexaﬂuoro-2-propanol(HFIP)-water mixtures. The phase diagrams obtained for the HFIP-water-amide
ternary systems at 298 K have shown aclosed-circle region of phase separation,and the more hydrophobic the amides, thelarger the region of phase separation.
To clarify the mechanism of amideinduced phase separation of HFIPwater mixtures, in the present study,
SANS experiments have been made on
HFIP-water-amide mixtures with threedifferent amides, N-methlyformamide(NMF), N-methylacetamide (NMA), andN-methylpropionamide (NMP). The hydrophobicity of the amides is larger in theorder of NMF < NMA < NMP.
HFIP-D2O-amide ternary solutions below
the lower critical composition and above
the upper critical one were prepared in accordance with the phase diagrams. SANS
measurements at 298 K were made on thesample solutions by using the SANS-U
spectrometer with the camera lengths of 1
and 4 m. The scattering intensities were accumulated on the detector at the camera

lengths of 1 and 4 m for 10 min and 1 h per
sample, respectively.
Fig. 1(a) shows the Ornstein-Zernikecorrelation lengths xi estimated from the
SANS intensities for the HFIP-D2O-amide
mixtures below the lower critical composition as a function of amide mole fraction. For each amide system, the xi value
increases with increasing amide mole fraction. It is suggested that the heterogeneity of the mixtures increases with the increase in the amide concentration toward
the critical one. The NMP system requires
the smallest amount of amide to enhance
the heterogeneity among the systems. Fig.
1(b) shows that the amide mole fraction
dependence of the xi values for the HFIPD2O-amide mixtures above the upper critical composition. The xi value for each system gradually decreases when the amide
concentration increases apart from the critical one. The NMP system requires thelargest amount of amide to recover the homogeneous mixing.
Below the lower critical composition, a small amount of amide added
may be easily solvated by hydrophobic
HFIP molecules rather than water ones,
resulting in the enhancement of HFIP
clusters around amide molecules. Hence,phase separation occurs when clusters are
evolved to a macroscopic size. Above thelower critical composition, on the contrary, amide molecules further added may
play a role as an interface between HFIP
and water clusters because of the amphiphilicity of amide molecule, i.e., HFIP,
water, and amide molecules are homogeneously mixed again. Thus, the HFIPwater-amide systems reveal a closed-circle
region of phase separation, and the region for the HFIP-water-NMP system is thelargest among the three systems due to themost hydrophobic NMP.

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JAEA-Review 2011-050[1] K. Yoshida, M. Misawa, K. Maruyama,
M.; Imai M. Furusaka, J. Chem. Phys., 113,2343-2348 (2000).
[2] T. Takamuku, D. Matsuo, A. Yamaguchi,
M. Tabata, K. Yoshida, T. Yamaguchi, M.
Nagao, T. Otomo and T. Adachi, Chem.
Lett., 2000, 878-879.
[3] T. Takamuku, A. Yamaguchi, D. Matsuo, M. Tabata, M. Kumamoto, J. Nishimoto, K. Yoshida, T. Yamaguchi, M. Nagao,
T. Otomo and T. Adachi, J. Phys. Chem. B,
105, 6236-6245 (2001).
[4] T. Takamuku, Y. Noguchi, E. Yoshikawa,T. Kawaguchi, M. Matsugami and T.
Otomo, J. Mol. Liquids, 131/132, 131-138(2007).

Fig. 1. Xi values for HFIP-water-amide mixtures (a)below the lower critical composition and (b) above
the upper critical one as a function of amide mole
fraction.

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JAEA-Review 2011-050

1-4-5
Alkyl-chain Dependence on Micro-phase Separation of Room Temperature Ionic
Liquids
Kenta Fujii (A), Yasuhiro Umebayashi (B), Shin-ichi Ishiguro (B), and Toshiyuki
Takamuku (A)(A) Saga Univ., (B) Kyushu Univ.
Room temperature ionic liquid has
attracted attention as a new solvent ofnegligible vapor pressure and incombustibility. Recently, it has been reported
by simulation and thermodynamic studies[1,2] that nonpolar (alkyl-chain group)and polar (cationic imidazolium ring
and anion) domains are formed in 1alkyl-3-methylimidazolium(C(n)mim+)hexaﬂuorophosphate ionic liquids with thealkyl-chain length longer than n = 4, thus
micro-phase separation occurs in the ionicliquids. In this work, small-angle neutron
scattering (SANS) measurements for the
C(n)mim+ bis(triﬂuoromethanesulfonyl)
amide (TFSA-) were carried out at 298
K to elucidate experimentally the effectof varying the alkyl-chain length on the
micro-phase separation.
SANS measurements were made on theC(n)mim+TFSA- (n = 2, 4, 6, 8, 10 and 12)
by using SANS-U spectrometer with thecamera length of 1 and 4 m. The scattering intensities for the sample liquids wereaccumulated on the detector at the camera
lengths of 1 and 4 m for 10 min and 1 h,
respectively.
Figure 1 shows SANS spectra obtained for
the C(n)mim+TFSA- with the alkyl-chain
length from 2 to 12. The SANS proﬁlesfor all the ionic liquids at low Q region
do not show the Orstein-Zernike behavior. Indeed, a peak appears in the range of
0.15 < Q/A-1 < 0.35 with increasing thealkyl-chain length and shifts to lower Q
side. A peak ﬁtting using Lorentzian function was performed on the SANS spectra,
as shown by solid line in Fig. 1, to obtain
the peak position Q0, and then the spatial correlation (= 2pi/Q0) were estimatedto be 15, 22 and 26 A for n = 8, 10 and
12, respectively. The spatial correlation ob-

viously depends on the alkyl-chain length,
indicating that the alkyl-chain groups aggregate to form domains or clusters in theionic liquids with n = 8 up to 12, but do
not aggregate with n = 2 to 6. Here, according to our large-angle high-energy Xray scattering measurements, it has foundthat the carbon - carbon interactions among
the alkyl-chain groups of the C(n)mim+
strengthen with increasing n. This is consistent with the present SANS results, i.e., theexperimental evidence for the long-rangeordering of room-temperature ionic liquids
at the molecular level.
References[1] J. N. A. C. Lopes, A. A. H. Padua, J.
Phys. Chem. B 110, 3330-3335 (2006)[2] L. M. N. B. F. Santos, J. N. C. Lopes, J.
A. P. Coutinho, J. M. S. S. Esperanca, L. R.
Gomes, I. M. Marrucho, L. P. N. Rebelo, J.
Am. Chem. Soc. 129, 284-285 (2007)

Fig. 1. SANS proﬁles of C(n)mim+TFSA- ionic liquids

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1-4-6
Structural Change of Supercritical Carbon Dioxide with Entrainer Molecule
T. Sato A , M. SugiyamaB , M. MisawaC , K. Hamada A , K. ItohB , K. MoriB , and T.
FukunagaB
A Grad. Sch. Eng. Kyoto Univ., B KUR, Kyoto Univ., C KEK
Recently, supercritical carbon dioxide(sc-CO2 ) has attracted much attention as anenvironmentally accepted solvent. The solvent power of sc-CO2 extremely increases
with adding a small amount of entrainer
molecule such as alcohol, carbon hydride,
and water. Since the solubility of sc-CO2
is strongly connected with its ﬂuctuation
structure, it is quite important to investigate the effects of entrainer for mesoscale structure of sc-CO2 . In the present
study, the structural change of sc-CO2 induced by adding the entrainer has been observed with small-angle neutron scattering(SANS).
A SANS experiment was performed using SANS-U of the Institute for Solid State
Physics, the University of Tokyo installedat JRR-3M in Tokai, Japan. Scattering intensity with a Q range between 0.02 and
0.2 Å−1 can be measured by using 7 Åneutron in 2 m camera length. Methanol(CD3 OD) or ethanol (C2 D5 OD) was added
into sc-CO2 with 1 mol% concentration as
entrainer. Measurement temperature wasﬁxed at 38 ◦ C and pressure was varied from7.66 to 10.36 MPa.
The ovserved SANS intensity was simply analyzed with Ornstein-Zernike (OZ)
equation to obtain OZ correlation length, ξ,
and I (0). Although the system consistedof both density and concentration ﬂuctuations, all the SANS data can be well analyzed with a single OZ equation. Since theconcentration of entrainer was dilute, thescattering intensity mainly came from thedensity ﬂuctuation of the mixed solution.
The pressure dependences of ξ and I (0)along the isotherm are shown in Fig. 1(a)and 1(b), respectively. Results of both pureand alcohol entrained sc-CO2 are displayedin this ﬁgure. Each data has a maximum
along the isotherm corresponding to theridge structure in supercritical region. The
maximum values of ξ and I (0) of sc-CO2
with alcohol become considerably larger
than those of pure sc-CO2 . Moreover, thepressure at which the ﬂuctuation becomesmaximum sifts to the lower. It was suggested that these changes could be induced
by attractive interaction between the alcohol and CO2 molecules. Magnitude of
the interaction with the ethanol is stronger
than that with the methanol. It is considered that these structural changes with alcohol molecules associate with the increaseof solvent power of sc-CO2 .

Fig. 1. Change of structural parameters ξ and I (0)along the isotherm of 38 ◦ C induced by adding
1 mol% methanol and ethanol.

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1-4-7
Static and Dynamic Structure of Meso-scale ﬂuctuations in liquid chalcogens near
the metal-nonmetal transition
Y.Ohmasa, T.Hoshino R.Osada and M.Yao
Department of Physics, Graduate School of Science, Kyoto University[2] M. Yao, N. Itokawa, H. Kohno, Y. Kajihara and Y. Hiejima, J. Phys.: Condens.
Matter 12 (2000) 7323
0.6
oTe7Se3 + quartz cell 490 C

Q=0.046A
I(Q,t)/I(Q,0)

Liquid Te-Se mixtures exhibit a metalnonmetal (M-NM) transition in a relatively
narrow temperature range [1]. This transition is accompanied by anomalies in thermodynamic properties such as the thermal expansion coefﬁcient and compressibility. Recently, sound attenuation measurements for liquid Te-Se mixtures revealed that there occur dynamic anomalies
in the M-NM transition region [2]. From
the frequency dependence of the soundattenuation coefﬁcient α, their relaxation
time is estimated to be of the order of nanoseconds. These anomalies may be related
to the relaxation between the metallic andnon-metallic states in the liquid, and it isinteresting to study the space- and timestructure of the mesoscale ﬂuctuations.
In the present work, we studied the staticand dynamic structure of meso-scale ﬂuctuations in liquid Te-Se mixtures near the
metal-nonmetal transition by using Neutron Spin-Echo (NSE) and Small Angle
Neutron Scattering (SANS) techniques.
The closed and open circles in Fig.1
show the intermediate scattering function I ( Q, t)/I ( Q, 0) of Te7 Se3 sample ina quartz cell observed at Q =0.046A−1
and 0.064A−1 , respectively, at 490o C. These
data indicate that there exists a relaxation
process in the nsec region. In addition,from the SANS measurement, we observeda strong peak at Q ∼ 0.2A−1 for the liquid Te-Se mixtures for the ﬁrst time. This
peak may be related to the meso-scale ﬂuctuations in the M-NM transition region.

−1

0.4

0.2

Q=0.064A

0

0

2

4

−1

6

8

tF [nsec]
Fig. 1. Intermediate scattering function I(Q,t)/I(Q,0)
for liquid Te7Se3 in a quartz cell at 490C. The solidlines indicate the ﬁtting curves.

References[1] M. Yao and H. Endo, J. Non-Cryst.
Solids 205-207 (1996) 85, and references
therein.

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1-4-8
Small Angle Neutron Scattering Investigation of Aggregation of
N,N -dialkylamide and Its Eﬀect on Nitric Acid Extraction
S. Suzuki, T. Yaita1 , R. Motokawa2 and S. Koizumi2
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195
1
Quantum Beam Science Directorate, JAEA, Harima, Hyogo, 679-5148
2
Advanced Science Research Center, JAEA, Tokai, Ibaraki, 319-1195

In solvent extraction chemistry, this extractant aggregate with metal ions (likes uranium
and plutonium) and/or inorganic acid makes
heavy organic phase (it is called the third
phase) between an aqueous phase and an organic phase. This aggregate in the nuclear
spent fuel reprocessing causes serious problems, such as a criticality accident and inhibition of stable process operation. In orderto understand this aggregate with metal ionsand inorganic acid, the structure analysis ofhigh concentration metal ion and/or inorganicacid loaded organic phase as a reprocessing
process is required. However, large extractant aggregates or polymeric species are often
formed under reprocessing conditions, which
has not been studied in detail.
N,N -dialkylamide extractants strongly aggregate with uranium or nitric acid in
non-polar diluents has been reported3) .
SANS studies of the aggregation of N,N dihexyloctanamide (DHOA) dissolved indeuterated n-octane have been preformed.
The samples were made as following procedure, 2 ml of deuterated n-octane as an organic solvent containing 1.0 mol/dm3 DHOA
was shaken with the same volume of the various nitric acids (2.0, 4.0, 6.0, 9.0 mol/dm3 ).
After centrifugation this sample, 0.5 ml of theorganic solution was separated to use as asample. 0.5 ml of DHOA solution was en原子炉：JRR-3

装置：SANS-J(C3-2)

closed in Quartz cell. SANS measurement
were performed by the SANS-J instrumentwith λ=0.706 nm at the JRR-3M reactor in
JAEA. The scattering data of extracted samples were collected for 1 hour at room temperature.
Figure 1 shows the ﬁrst obtained scattering proﬁles of nitric acid (2.0, 4.0, 6.0, 9.0
mol/dm3 ) extracted DHOA samples.
In next step, data analysis for these results
should be carried out. Furthermore, SANS
measurement, vapor pressure osmometry, interfacial tension measurement for radioactive samples (uranium(VI) and thorium(IV))
should be investigated.
3

2.0 mol/dm HNO33

4.0 mol/dm HNO33

6.0 mol/dm HNO33

9.0 mol/dm HNO3Intensity

Small Angle Neutron Scattering (SANS)
is a powerful technique in structural studies of polymers and micelles1) . Recent studies have shown the applicability of the SANS
technique to solvent extraction chemistry2) .
SANS has ability to elucidate the size andthe shape of the extractant aggregates formed
upon metal cations and inorganic acid extraction.







5

6 7 8 9

2

3

4

5

0.01

6 7 8 9

2

3

0.1
-1

q (Å )

Figure 1: SANS curves of DHOA-nitric acid extracted
samples.

References
1) L.J.Magid :“Structure and Dynamics by SmallAngle Neutron Scattering, in nonionic Surfactants,
Physical Chemistry”, M.J.Schick Ed., Surfactant
Science Series, 23, Maercel Dekker, Inc., New York,(1987).
2) M.P.Jansen, T.Yaita, and R. Chiarizia :“Langmuir”, 23(9), pp. 4765 (2007).
3) G.M.Gasparini, and G. Grossi :“Solv. Extr, Ion
Exch.”, 4(6), 1233 (1986).

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1-5-1

Dynamical Study on Nanocomposite Hydrogelby Means of Neutron Spin Echo TechniqueHitoshi Endo, Sho Miyazaki and Mitsuhiro Shibayama
ISSP, The University of Tokyo“Nanocomposite” is a current key aspectfor development of advanced materials [1],e.g., polymer-clay nanocomposite in synthetic systems [2]. Recently, polymer-clay
nanocomposite hydrogels (NC gel) havebeen developed by Haraguch et al. [3, 4],which have extraordinary superior properties as large deformability with high elasticity, quick shrinkage after large deformation, non-destructivity, high optical transsparency, and so on. Since conventionalorganogels are very fragile, these characteristics of NC gels are great advantages formaterial use.
We have studied the static structure ofNC gel in detail by means of contrast variation SANS [5], and conﬁrmed that thepolymer chains are adsorbed on clay surface, then the clay nanoparticles work as 2dimensional cross-linkers.
In this study, dynamical property of thenanocomposite hydrogel was investigatedby means of neutron spin echo technique.
Since 10.8 Åwavelength neutron beam wasunsed for low Q region (0.04 ≤ Q[Å−1 ]≤ 0.07), the achieved maximum Fourier
time was a bit more than 40ns, while 7.3
Åwavelength neutron beam was unsed forhigh Q region (0.09 ≤ Q[Å−1 ] ≤ 0.2), sothat the maximum Fourier time was 15ns inthat case. Fig. 1 shows the measured normarized intermediate scattering functions
from the nanocomposite gel consisting of 4
vol% of polymer and 1 vol% of clay with
deuterated water. The curves in Fig. 1
show the ﬁtting results withI ( Q, t)= exp(−Γt)
I ( Q, 0)liquids, but do not decay exponentially at
longer Fourier time, which may be due tothe gel structure, i.e., the polyer gels aremacroscopically solids but microscopicallyliquids, and the polymers can ﬂow in shorttime scale but their center of masses arefrozen for longer time scale.
References[1] L. A. Utracki, Clay-Containing Polymeric
Nanocomposites (Repra Tech. Ltd., London,
2004).
[2] A. Okada and A. Usuki, Macromol. Mater.
Eng. 291, 1449 (2006).
[3] K. Haraguchi and T. Takehisa, Adv. Mater.
14, 1120 (2002).
[4] K. Haraguchi, T. Takehisa and S. Fan,
Macromolecules 35, 10162 (2002).
[5] S. Miyazaki, H. Endo, T. Karino, K.
Haraguchi, and M. Shibayama, Macromolecules 40, 4287 (2007).

Fig. 1. Normalized intermediate scattering functions I(Q,t)/I(Q,0) obtained from the nanocomposite hydrogel.

(1)

It is
at short Fourier times (< 5ns).
clearly shown that the measured intermediate scattering functions decay as like as
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1-5-2
Hysteresis of bicelle/ULV transition in long- and short-chain lipid mixture
Norifumi L. YAMADA, Naoya TORIKAIHigh Energy Accelerator Research Organization
phase opened to one bicelle with decreasing temperature. Therefore, bicelles after
annealing is larger than before annealing,
since some small bicelles fuse into one ULVat the ULV formation. This new histeresis would be a important help to understand the mechanism of the hysteresis of bicelle/ULV transition.
References[1] M.-P. Nieh et al., Biophys. J. 82 (2002) 2487.
[2] M.-P. Nieh et al., Langmuir 21 (2005) 6656.
[3] S. Okabe et al., J. Appl. Cryst., 38 (2005) 1035.
12

10

11

10

10

10

9

10

20°C

2.11 wt.%

8

50°C

7

20°C

10
10
I(q) [arb. unit]

In the aqueous solutions of dimyristoylphosphatidylcholine (DMPC) and dihexanoylphosphatidylcholine (DHPC) mixture, bilayered-micelle, so called bicelle,
were formed at low temperature. These bicelles fuse into large uni-lamellar vesicles(ULVs) above the chain melting temperature, Tc , of DMPC molecules (about 24◦ C)
when lipid membranes were charged [1].
Although these disk-fused ULVs usuallyﬁssure into small disk micelles below Tc ,the ULVs are stable even below Tc when thelipid concentration is very low [2]. However, the mechanism of the stable ULV formation has not been clariﬁed yet.
In this study, we observed the structure in the lipid mixture system below andabove Tc by SANS, and quantitatively discussed the stability of ULVs. The experiments were performed at 20◦ C and 50◦ C
with changing lipid concentration. DMPC
and DHPC were mixed in the molar ratio of [DMPC]:[DHPC] = 4.6:1, and dissolved in the D2 O solution of 3 mM CaCl2 .
The SANS experiments were carried out at
SANS-U, JRR-3M, JAEA, Tokai, Japan [3].
Figure 1 shows the temperature dependence of SANS proﬁle with changing
lipid concentration. While no hysteresis
was observed at high lipid concentration(2.11 wt.%), the SANS proﬁles at low lipid
concentration (0.35 wt.%) show the hysteresis as shown by previous study [2]: theproﬁle of bicelles at 20◦ C changed to ULVs
with increasing temperature up to 50◦ C,
and the proﬁle of ULVs remained even after decreasing temperature down to 20◦ C.
Although such the hysteresis was observed
even at intermediate lipid concentration(1.06 wt.%), large bicelles appeared insteadof ULVs after annealing. In this case, thevolume of bicelle evaluated by the ﬁtting
is almost same to that of ULV shell. Thismeans that one ULV at high temperature

6

10

5

10

20°C

1.06 wt.%

10

4

50°C

3

20°C

10

2

10

1

10

20°C

0.35 wt.%

0

10

50°C

-1

10

20°C

-2

10
2
0.001

4 6 8

0.01

2

4 6 8
-1

0.1

2

4 6 8

1

q [Å ]

Fig. 1. Temperature dependence of SANS proﬁlewith changing lipid concentration. Temperature sequence is indicated by the arrows.

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1-5-3
Changes in ﬂow-induced aggregated structures of shear-thickenning silica
suspensions
M. Ando (A), H. Mizukawa (A), Y. Takahashi (B), and M. Kawaguchi (A)(A) Mie University, (B) Kyushu University
In this report, we performed small-angle
neutron scattering (SANS) under shear
for the 4.93 vol% fumed hydrophobic silica particles, whose surface is chemicallycoated by dimethyl n-hexadecane silicone,
suspended in dioxane and n-hexadecane.
The wavelength was selected to be 0.7 nm.
The suspensions pre-conditioned by a debubbling mixer were transfered to a quartz
co-axial rheometer cell with the gap lengthof 1 mm. The sample to detector distanceswere 4 m and 12 m. The resulting scattering
intensity was normalized to the isotropic
scattering intensities of the respective dispersants after substraction of the background due to the corresponding dispersants. The SANS experiments were performed under applied shear rates ranged
from 0 to 600 1/s at 27 oC.
The rheological measurements of thecorresponding silica suspensions were performed using a commercial rheometer ofMCR-300: rheochaos response, namely irregular time variation in the stress/shear
rate at a constant shear rate/stress arising from nonlinearities in the viscoelastic
constitutive equations, was observed forthe silica suspension in dioxane at limitted shear rates, whereas such a response
was not detective for the silica suspensions
in n-hexadecane during the shear rates
examined. Similar rheochaos responses
were observed in several soft matters, suchas worm-like micelle solutions, lamellar,
onion, and sponge phases of surfactants,
and dense colloidal suspensions.
Figure 1 shows a double logarithmic plotsof the scattering intensity (I(q)) as a function of the wave vector (q) for the silica suspesnion in dioxane. The values of I(q) apparently superimpose on the same curve,
irrespective of the shear rate. The respective log-log plots of I(q) versus q scale lin-

early a slope of - 2.0 below q = 0.2 1/nm
and - 4.0 above this q value, where theI(q) tends toward Porod’s law. The former
slope corresponds to the mass fractal dimension (Dm) for the aggregated objects,
while the latter slope gives the surface fractal dimension (Ds) according to the relationship, I(q)˜ qˆ- (6-Ds), leading to the Ds
value of 2.0. The resulting Ds value issmaller than that for the hydrophobic R202
silica particles, whose surface is chemicallycoated by silicone oil with the degree ofpolymerzation of 6 in trans-decalin. Moreover, the q value intercected between theslopes of - 2.0 and - 4.0 gives the size of the
primary silica particle and leads to 11.5 nm,
which is almost equivalant to the diamaterof the corresponding fumed silica. However, we can notice that the magitude of theI(q) vales at the shear rate ranges from 20
to 300 1/s where rheochaos response is observed, is clearly larger than that without
rheochaos response by the plots of I(q) as afunction of log q.
On the other hand, the scattering curves
for the silica suspensions in n-hexadecane
can be much better superimposed thanthose in dioxane, irrespective of the applied shear rate. This means that changes
in the scattering intensities are not clearlyobserved when shear rate is varied. However, the difference between the scattering
curves of the silica suspensions in dioxane
and n-hexadecane was observed at the qvalues higher than 0.1 1/nm, where the former scattering intensity was clearly larger
than the latter one if both scattering curves
in dioxane and n-hexadecane at lower q regions were supperimposed.
In conclusion, this SANS experimentshows that the rheochaos response is wellcorrelated with the changes in the scattering curves and the fractal strucures of the

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silica suspensions can not be easily broken
out by the applied shear rates.

Fig. 1. SANS scattering curves of the silica suspensions in dioxane under the applied shear rates.

1-5-3

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1-5-4

Simultaneous Evaluation of Lipid Exchange and Flip-Flop in Vesicles
Nakano(A), M. Fukuda(A), T. Kudo(A), H. Endo(B)(A)Graduate School of Pharmaceutical Sciences, Kyoto Univ., (B)ISSP-NSL, Univ. of Tokyo
We recently succeeded in determining the rates of interbilayer exchange
and ﬂip-ﬂop of dimyristoylphosphatidylcholine (DMPC) in large unilamellar vesicles (LUVs) by small-angle neutron scattering (SANS) technique [1]. This techniquetakes advantage of the large difference inthe scattering length density between hydrogenated and deuterated lipids, and theexchange of these lipids between LUVs results in a decrease in the scattering intensity, which can be detected by timeresolved SANS (TR-SANS) measurements.
In this study, effect of cholesterol (Chol)on the rate of interbilayer and transbilayertransfers of DMPC was evaluated by TRSANS measurements.
DMPC, d54-DMPC, were obtained from
Avanti Polar Lipids Inc. (Alabaster, AL).
Cholesterol (Chol) was from Sigma (ST.
Louis, MO). LUVs consisting of deuterated (D-LUV) or hydrogenated DMPC (HLUV) and Chol (0, 20, and 40 mol% of total
lipids) with a diameter of ca. 100 nm wereprepared by extrusion method using Trisbuffered saline prepared from mixtures of
D2O and H2O. LUVs consisting of 1:1 mixture of deuterated and hydrogenated lipids(D/H-LUV) were also prepared by mixing
these lipids and Chol before hydration. Volume fraction of D2O in the Tris-buffer was
0.5, 0.45, and 0.4 for LUVs with 0, 20, and40 mol% Chol, respectively, which corresponds to the contrast-matching condition
between D/H-LUV and solvent. Phospholipid concentration of each LUV preparation was set to 20 mM. SANS measurements were performed at 37 °C using
SANS-U with 7 angstrom of incident neutron beam. Sample-to-detector distance
was set to 4 m.
First, we conﬁrmed that D-LUV and HLUV had almost identical scattering proﬁle, while D/H-LUV exhibited little scat-tering at the contrast matching condition.
TR-SANS measurement was started immediately after mixing equivalent volumeof D-LUV and H-LUV. Time-course of thenormalized contrast was calculated fromthe scattering intensity and plotted in Figure 1. The contrast decay proﬁles dependon the mole fraction of Chol. In the absence of Chol, the normalized contrasts
reached below 0.5, suggesting an involvement of ﬂip-ﬂop, and the obtained contrast
decays were well reproduced by the kinetic
model that takes account of both the interbilayer and transbilayer exchange. Theseexchange rates were reduced in the presence of Chol, and the ﬂip-ﬂop was vanished at 40 mol% Chol, where lipids are
known to form liquid-ordered phase.

Fig. 1. Contrast decays of DMPC/Chol LUVs with 0(circles), 20 (squares), and 40 mol% Chol (triangles)
after mixing D- and H-LUV at 37 °C.

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1-5-5Structure Analyses of Nanoemulsion/polymer Mixtures Having Dilatancy Behavior
M. Shibayama A , Y. KawadaB , T. KumeB ,H. Endo A ,N. Osaka N. A ,T. Matsunaga A
A ISSP-NSL, University of Tokyo
B Beauty Care Res. Lab., Kao Co., Ltd.
The microscopic structure of shearinduced gels for a mixed solution of
2-hydroxyethyl cellulose (HEC) andnanometer-size spherical droplets (NE) has
been investigated by in-situ small-angle
neutron scattering (SANS) with a Couettegeometry as a function of shear rate, γ̇.
The following facts were disclosed.
(1) There is a suitable range of NE andHEC concentrations necessary for a shearinduced sol-gel transition. The size of thepolymer chains needs to be comparablewith the inter-particle distance, a, of the oildroplets in NE. (2) In the stationary state,
the polymer chains do not bridge neighboring droplets and are localized to one ora few droplets via weak molecular interaction, such as van der Waals interaction
and/or hydrogen bond. (3) Nanodroplets
are dispersed in the solution with the electrostatic repulsive interaction and keep theinter-particle distance. (4) With increasingγ̇, the viscosity increased rapidly at γ̇  4.0
s−1 , followed by a shear thinning. After
cessation of shear, the system exhibitedan extraordinarily large steady viscosity.
This phenomenon was observed as a shear
induced sol-gel transition. (5) Real-time
SANS measurements showed an increasein the scattering intensity exclusively at
low scattering angle region. However,neither orientation of polymer chains nor
droplet deformation was detected andthe SANS patterns remained isotropic
irrespective of γ̇. It took about a few
days for the gel to recover its original sol
state. (6) Shear-induced sol-gel transition
occurs when the system is percolated with
deformed polymer chains via droplets. (7)For systems having highest dilatancy ratio,
the shear stress at the transition σtr is simply estimated by the interparticle distance,a, i.e., σtr ≈ kB T/a3 , and is independentof the molecular weight of the polymer,
where kB and T are the Boltzmann constantand the absolute temperature, respectively.
This means that the shear (or shear rate)necessary for the transition is of the order of unity, i.e., γtr ≈ 1. (8) The shear
thickening is not necessarily ascribed to a
non-Gaussian chain deformation, such as
an inverse Langevin chain conformation,
but to a Gaussian chain statistics witha ﬁller-assisted percolation. A possible
mechanism of gelation is proposed fromthe viewpoint of shear-induced percolationtransition.1
References[1] M. Shibayama, H. Kawada, T. Kume, T.
Matsunaga, H. Iwai, T. Sano, N. Osaka, S.
Miyazaki, S. Okabe, and M. Shbayama, J.
Chem. Phys. 127, 144507-1-7 (2007).

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1-5-6
Ionic Strength Dependence of Chain Conformation of Hydrophilic Polymers at
Water Interface
M. Kobayashi1, Y. Terayama2, N. Hosaka2, A. Takahara*1,2
1Institute for Materials Chemistry and Engineering, 2Graduate School of Engineering, Kyushu
University
In general, an isolated polyelectrolyte inpure water forms a relatively expanded
state due to the electrostatic repulsion ofionic functional groups in the chain, while
it would shrink in salt solution by the reduction of electrostatic repulsion between
polymer chains. However, the inﬂuenceof the ionic strength on a dimension of
charged polymers should largely dependon chain ﬂexibility and environment. Polymer brush, for example, is the densely tethered polymer chains on a solid substrate
through the covalent bonds.[1] Brush layer
in a solution affords unusual high concentration of polymer and high osmotic pressure, resulting in a fairly extended conformation of the brush chains. In this study,
interface structure of surface-grafted polyelectrolyte brush at aqueous solution containing a salt was analyzed by neutron reﬂectivity (NR) measurements.
High-density polyelectrolyte brushes onquartz were prepared by surface-initiatedatom transfer radical polymerization of 2methacryloyloxyethyl phosphorylcholine(MPC) [2] and N,N-dimethylaminoethyl
methacrylate, which was transformed to 2(methacryloyloxy)ethyltrimethylammonium
iodide (META). NR measurements werecarried out with the multilayer interferometer for neutrons (MINE), using
wavelength of 0.88nm. Neutron beamirradiated from quartz to the interface
between heavy water and swollen brushon quartz glass. Scattering length density
proﬁles of PMETA brush in heavy water
calculated from the reﬂectivity curvesindicated that the PMETA chains werestretched up to 70 nm in heavy water
forming concentration gradient of heavy
water. Interestingly, quite similar reﬂective
curve was observed from the interface of

PMETA brush at 1.0 M of NaCl deuterium
oxide solution. Salt ion cannot be diffused
into a high-density polymer brush layer
due to the high osmotic pressure andhigh local charge density. Therefore, thethickness of PMPC brush in solution was
supposed to be hardly changed even ina salt solution. Similar results in anothertype of polyelectrolyte have also been
discussed by Matsuoka[3] and Kurihara[4]using X-ray reﬂectivity and surface-force
measurement, respectively.
References[1] W. J. Brittain et al, Polymer Brushes,
Wiley-VCH, Weinheim (2004).
[2] M. Kobayashi, Y. Terayama, N. Hosaka,
M. Kaido, A. Suzuki, N. Yamada, N.
Torikai, K. Ishihara, A. Takahara, Soft Matter, 3, 740 (2007).
[3] P. Kaewsaiha, K. Matsumoto, H. Matsuoka, Langmuir, 20, 6754 (2004).
[4] S. Hayashi, T. Abe, N. Higashi, M. Niwa,
K. Kurihara, Langmuir 18, 3932 (2002).

Fig. 1. Figure 1. Scattering length density proﬁles of
PMETA and PMPC brush in D2O and 1.0 M NaClsolution.

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JAEA-Review 2011-050

1-5-7

Surface and Interface Structure Analysis of (Multi-functionalized
Silsesquioxane/Deuterated Polystyrene) Hybrid Thin Films
N. Hosaka1, Y. Terayama1, M. Kobayashi2, A. Takahara*1,2
1Graduate School of Engineering, 2Institute for Materials Chemistry and Engineering, Kyushu
University
Polymer thin ﬁlms have gained much interest because of their numerous technological applications, however, producing stableand defect-free ﬁlms is problematic since
the polymer thin ﬁlms tend to break up
and dewet from a substrate. Previously,
it was shown that the addition of polyhedral oligomeric silesequioxane (POSS)
nanoﬁller stabilized the polystyrene (PS)thin ﬁlm against dewetting [1]. POSS,
which is characterized by the formula of(RSiO1.5)8, has a nanosized cage structurewith a silica core and organic groups on its
surface. The dispersion state of POSS in theﬁlm seemed to be an important factor tounderstand the ﬁlm stabilization effect [2],and the systematic study using designed
nanoﬁllers to control its dispersion state isa challenge for further development of thistechnique.
The present work is focused on the controlof the dispersion state of POSS nanoﬁllers
in PS thin ﬁlms through the introductionof the several substituents onto POSS surface. The dispersion states of the surfacemodiﬁed POSS in deuterated PS (d-PS)
thin ﬁlms were investigated by neutron reﬂectivity. Figure 1 shows the depth proﬁle models of scattering length density(b/V) of ca. 130 nm thick d-PS ﬁlm and
POSS/d-PS (10/90, w/w) ﬁlms. POSS withphenethyl groups (PhPOSS) was homogeneously dispersed into d-PS ﬁlm because of
the high afﬁnity of phenethyl groups withd-PS. The b/V of the ﬁlm was decreasedby the addition of PhPOSS compared withd-PS ﬁlm. In contrast, POSS having sevencyclopentyl groups and a low energy ﬂuoroalkyl group (CpPOSS-Rf) strongly segregated to the ﬁlm surface and formed thinlayer with low b/V. The difference of thesurface energy between CpPOSS-Rf and d-

PS provides a driving force for the segregation of CpPOSS-Rf to the ﬁlm surface. The
formation of low b/V layer was also observed at the surface and ﬁlm?substratet interface of d-PS ﬁlm containing POSS withseven cyclopentyl groups and a dihydroxylpropyl group (CpPOSS-2OH). CpPOSS2OH segregated to the surface and the interface of the ﬁlm because of the lower
surface energy of cyclopentyl groups thanthat of d-PS and the afﬁnity of the hydroxyl groups with the substrate, respectively. These results revealed that the dispersion state of POSS can be controlled bytuning the surface substituents on POSS,and expected to contribute to the design ofthe polymer thin ﬁlm properties by the addition of nanoﬁllers with controlled structures.
References[1] N. Hosaka, K. Tanaka, H. Otsuka,
A. Takahara, CompositeInterfaces, 11, 297(2004).
[2] N. Hosaka, N. Torikai, H. Otsuka, A.
Takahara, Langmuir, 23, 902 (2007).

Fig. 1. Figure 1. The depth proﬁle models of b/V ofd-PS ﬁlm and POSS/d-PS (10/90, w/w) ﬁlms near(a) the surface and (b) the ﬁlm?substrate interface.

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JAEA-Review 2011-050

1-5-8
Thermal ﬂuctuation of a lipid bilayer in the anomalous swelling regime
Hishida M., Seto H., Yamada N.L.
Department of Physics, Kyoto Univ.
Biomembrane is mainly composed of aphospholipid bilayer, which is spontaneously formed by mixing of lipid andwater. A various kinds of physical andchemical properties of phospholipid bilayers have been investigated, and a number of applications have been provided.
Spontaneously formed structure of phospholipid by mixing with water is multilamellar vesicles, while living cell membranes are uni-lamellar vesicles. It is important to understand the formation of cell
membrane self-organization of lipid bilayers in context with the interactions between
bilayers such as van der Waals interaction,
hydration repulsion and steric repulsion by
thermal ﬂuctuation of bilayer.
In order to understand interactions of lipid
bilayers, we focused on a phenomenon
called anomalous swelling [1]. In theanomalous swelling regime, i.e., temperature just above the main transition temperature from the liquid-crystalline phase to
the gel phase, the repeat distance between
stacked bilayers increase drastically. The
driving force for the increase has been considered to be ampliﬁed steric repulsion due
to the softening of lipid bilayer [2]. However, the softening is not conﬁrmed enoughespecially by microscopic picture, and themechanism of anomalous swelling is under
dispute.
In the present experiment, we performed
neutron spin echo spectroscopy (NSE)for the lipid bilayers in the anomalous
swelling regime at iNSE, JRR-3, JAEA. Bothmulti-lamellar vesicles and uni-lamellar
vesicles of DMPC were measured in thesame condition. Figure 1 shows the typical intermediate correlation functions of
DMPC small uni-lamellar vesicles. The
bending modulus of lipid bilayer is calculated using the theory by Zilman andGranek, and the values exhibit that bilayers

become harder in the anomalous swelling
regime. The same tendency is observedin the case of multi-lamellar vesicles. Thistendency is reasonable since the hydrocarbon chain of lipid molecules freeze inthe gel phase. The value of the bending
modulus estimated from the experiment is
two orders of magnitude larger than kT.
This result suggests that static disordering of stacking of bilayers such as metastable ripple phase is induced just above
the main transition temperature, and themulti-lamellar structure is swollen.
[1]J. F. Nagle et al., Phys. Rev. E 58 7769
(1998)[2]N. Chu et al., Phys. Rev. E 71 041904(2005)

Fig. 1. Intermediate correlation functions of DMPC
small uni-lamellar vesicles at 25 C and 38 C. Opencircles are the data from NSE and solid lines are ﬁtting results by Zilman and Granek theory.

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JAEA-Review 2011-050

1-5-9

Melting and Re-crystallization Process of Shish-kebab Structure
Go Matsuba, Yuji Hayashi, Chie Ito, Koji Nishida, Toshiji Kanaya
Institute for Chemical Research, Kyoto University
When polymer are crystallized under elongational or shear ﬂows, the so-called shishkebab structure could be observed. The
shish-kebab structure consists of long central ﬁber core (shish-structure) and lamellar crystal (kebab structure) periodically attached along the shish-structure and surrounded by the shish-structure. We studied the hierarchic structure of the shishkebab structure using three neutron spectrometers [1].
In the present experiment, we carried out
the time-resolved small angle neutron scattering (SANS) measurements on melting
and re-crystallization processes of shishkebab structure with hand-made temperature cell [2]. The initial shish-kebab structure was made from drawing blends ofdeuterated low molecular weight components and protonated ultra-high molecular weight polyethylene (PE) at 150 C.
The molecular weight of low molecularweight deuterated and protonated ultrahigh molecular weight PE (dPE/hPE) is
56,500 and 2,000,000. The SANS measurements were performed on SANS-U spectrometer on JRR-3M, JAEA, Tokai, Japan.
We observed temperature change of theshish-kebab structure during the heatingprocess from room temperature to above
the melting temperature and then quenching it to room temperature.
Figure 1 shows that 2D-SANS images atvarious temperatures during the heatingprocess and after quenching. In the heatingprocess, the position of spot-like scattering parallel to the drawing direction shifts
to lower angle. This result suggests the
spacing of kebab structure grows larger.
The kebab structure melts at 133 C. Whenthe sample was heated up 180 C above
the melting temperature, the shish-kebab
structure was not observed after quenching to room temperature, but the isotropic

crystal morphology was shown as in Figure1(a). However, as seen in Figure 1(b), when
the sample was molten at 136 C and thenquenched to room temperature, the shishkebab structure appeared again. These results suggest that the melt of PE blends
on 180 C is isotropic, on the other hand,some oriented structure in melt is reserved at 136 C. For detailed analysis, weevaluated the scattering proﬁles normal tothe drawing direction in order to clarify theshish-structure melting process. The scattering intensity in lower q-range below 0.15
Aˆ-1 vanished at about 138 C, while thatof higher q-range above 0.15Aˆ-1 still remained at141 C.
References[1] T. Kanaya et al., Macromolecules, 40,3650, 2007.
[2] K. Nishida et al., Activity Reports on
Neutron Scattering Research, ISSP, U ofTokyo, 13, 2006.

Fig. 1. Temperature dependence of 2D SANS proﬁles for melting and recrystallization process ofshish-kebab.

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JAEA-Review 2011-050

1-5-10Gelation Mechanism of Clay-Polymer Nanocomposite Hydrogel using Contrast
Variation SANS
Shibayama M. A , Miyazaki S. A , Endo H. A , Karino T. A , Haraguchi K.B
A ISSP-NSL, University of Tokyo B Kawamura Institute of Chemical Researchintensities of Fig.1(a) by singular value
decomposition. In order to check the validity of decomposition, the reconstructed
scattering intensities are added in Fig.1(a)with solid line. Comparing these scattering intensities, the decomposition was
successful. The most important result isthat the sign of SCP (q), which corresponds
to the clay-polymer cross-correlation, is
positive. It indicates that there are spatial
cross-correlation between clay and polymer. Then we assumed that clay platelets
are surrounded by polymer layers andthese surrounded clay platelets are tiedby polymer network. Thus we calculated
the scattering function from this modeland we can successfully ﬁt these partial
scattering functions. From the ﬁtting, clay
platelets are surrounded by polymer layers, whose volumes are about 2.5 times of
the clay platelets. Furthermore, this model
represented the scattering functions of theother samples, regardless of gel and sol. It
indicates that the microscopic structures ofNC gel are almost identical regardless ofgel and sol.
[1] K. Haraguchi and T. Takehisa, Adv.
Mater. 14, 1120 (2002).
(a)

(b)
10
10-21

Sij / cm3

1

I(q) / cm-1

Recently, clay-polymer nanocomposites have been focused much attention because of their excellent physicalproperties. Haraguchi et al. reported
a novel clay-polymer nanocomposite gels (NC gels) consisting of synthetic hectorite (Laponite) and poly(Nisopropylacrylamide) (PNIPA)[1].
This
NC gel has excellent physical properties,
such as toughness, large deformability,
large swelling ration, rapid shrinking capability, and high transparency. We carriedout structure investigation of NC gelsof various concentrations by small-angle
neutron scattering using contrast variation
technique (contrast-variation SANS) in
order to learn the gelation mechanism.
We prepared NC gels of four different
concentrations, two dense samples were ingel state and two dilute samples remained
sol state. Investigating the microscopic
structures of these samples near galationthreshold, we can learn the galation mechanisms of NC gels. Since NC gel is a threecomponents system, consisting of clay,
PNIPA, and water, the scattering intensity is given by clay-clay, clay-polymer,
polymer-polymer correlations. Thus using
water of more than three different scattering length densities, we can decompose
the scattering intensities into their partial
scattering functions. In this case, we used
contrast controlled water with different
D2 O fraction.
Fig.1(a) shows the scattering intensitiesof the most dense sample and the partial
scattering functions. Scattering intensityof NC gel is minimum in the case of D2 O
fraction was 56%. With increasing D2 O
fraction, the scattering intensity became
large. Fig.1(b) shows the partial scatteringfunctions obtained from the scattering

0.1

fD2O = 0
fD2O = 0.56
fD2O = 0.66
fD2O = 0.76
fD2O = 1.0
reconstructions

0.01

7 8

0.01

2

3

4

-1

q/Å

10-22

10-23

SCC(q)SPP(q)SCP(q)

10-24
5 6 7 8

0.1

7 8

0.01

2

3

4

-1

5 6 780.1

q/Å

Fig. 1. (a)Scattering intensities and (b)obtained partial scattering functions.

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JAEA-Review 2011-050

1-5-11

Structural Formation Process under Drawing
Koji Nishida, Toshiji Kanaya, Go Matsuba, Yuji Hayashi, Chie Ito
Institute for Chemical Research, Kyoto University
Crystallization of polymers under drawing has been extensively investigated because drawing process quite affects theproperties and strength of ﬁbers and plastics. When polymers crystallize underdrawing, the so-called shish-kebab structure could be observed. The shish-kebab
structure consists of long central ﬁber core(shish-structure) and lamellar crystal (kebab structure) periodically attached along
the shish-structure and surrounded by theshish-structure. It is believed that the shish
structure is formed by completely stretchedpolymer chains and the kebabs are folded
chain lamella crystals and grow to the direction normal to the shish-structure. In
previous paper, we have revealed the hierarchic structure of the shish-kebab in awide special scale using three kinds of neutron spectrometers [1].
In the present experiment, we carriedout the time-resolved small angle neutron scattering (SANS) measurements on
structural formation processes of blendsof deuterated polyethylene and ultra-highmolecular weight protonated polyethylene(dPE/hPE) with the hand-made shear cell[2], which was modiﬁed to observe drawing processes in this experiment. The rangeof drawing rate is from 6 micron/s to
7.2 mm/s. We employed a large torquemotor with a maximum load capacity of
about 3.5 Nm and then could draw very
rigid sample. Polymer crystallization experiments require precise temperature control. Hence, the temperature was controlled within 0.3 C in a range from room
temperature to 200 C. The maximum
drawing ratio is about 5 in normal setting. The SANS measurements were performed on SANS-U spectrometer on JRR3M, JAEA, Tokai, Japan.
Figure 1 shows 2D SANS images during
the drawing process at 125 C. Before draw-

ing, we could observe only isotropic scattering from spherulites or isotropic lamella.
In the beginning, the scattering proﬁles
look like ellipsoid because the long period spacing increases in a direction parallel to the drawing, and then they become
two spots patterns. Now we are analyzing
the shish-kebab structure formation process during the drawing process at various
crystallization temperatures.
References[1] T. Kanaya et al., Macromolecules, 40,3650, 2007.
[2] K. Nishida et al., Activity Reports on
Neutron Scattering Research, ISSP, U ofTokyo, 13, 2006.

Fig. 1. 2D SANS images during drawing process annealed at 125 C.

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JAEA-Review 2011-050

1-5-12Distribution of glass transition temperature in polymer thin ﬁlms by neutron
reﬂectivity
Inoue R1 , Ogawa H1 , Kanaya T1 , Nishida K1 , and Hino M2
Institute for Chemical Research, Kyoto University1 , Reserch Reactor Institute, Kyoto
University2With the recent progress of evaluation
methods for polymer thin ﬁlms, it was
found that the physical properties of polymer thin ﬁlms were very different fromthose of bulk state. Among them, thickness
dependence of glass transition temperature(Tg ) is one of the most attractive topics andthe decrease of Tg with thickness was observed for polystyrene (PS) [1-3]. The singularity of Tg behaviour of polymer thinﬁlm is now understood in terms of multilayer or heterogeneous structure, however
the deﬁnite mechanism of glass transitionin polymer thin ﬁlms is still missing. In order to reveal the mechanism of glass transition of polymer thin ﬁlms, we have to
study multi-layer structure of polymer thinﬁlms in more detail. We studied the distribution of glass transition temperature inpolymer thin ﬁlms using multi-layered thinﬁlm by stacking hydrogenated PS (h-PS)
and deuterated PS (d-PS) with neutron reﬂectivity. Neutron can discern h-PS layerand d-PS layer clearly due to the differenceof neutron scattering length density, hence
we can evaluate Tg at a given position. We
used h-PS with molecular weight (Mw ) of
769K and molecular weight distributions(Mw /Mn ) 1.18 and d-PS with Mw of 731K
and Mw /Mn of 1.08 and we prepared dPS/h-PS/d-PS tri-layered thin ﬁlm. In order to minimize the effect of inter-layer diffusion between h-PS layer and d-PS layer,
we annealed this tri-layered thin ﬁlm at
365K that is about 10K below bulk Tg for 12
h. The neutron reﬂectivity measurements
were done with MINE-II reﬂectometer installed in JRR-3M reactor and the measurements were performed from 298K to 403K
in a vacuum cell. Figure 1(a) indicates theneutron reﬂectivity proﬁles from d-PS/h-

PS/d-PS tri-layered thin ﬁlms at 298K and
403K. Solid and dashed curves are the results of ﬁt using a three-layer model withthe formula derived by Parratt. The agreements of the ﬁts are very good for both
below and above bulk Tg , therefore weused three-layer model for the evaluationof ﬁlm thickness and roughness of eachlayer. Temperature dependence of thickness of each layer is shown in Figure 1(b).
At low temperature, thickness began to increase due to the thermal expansion, however thickness began to shrink at around360K. It was supposed that this was causedby the unrelaxed structure of polymer thinﬁlm due to lack of annealing. Kanaya et al.
reported that Tg value of polymer thin ﬁlm
was not affected by annealing condition [4],hence we evaluated Tg of each layer fromthe intersection of solid lines, as shown byarrows in Figure 1 (b). The evaluated Tgof each layer from top to bottom is 363K,
390K, and 383K, respectively. Although wehave to study the annealing effect in order
to disclose the distribution of Tg in polymer
thin ﬁlms, we could roughly withdraw the
distribution of Tg in polymer thin ﬁlm.
References [1] J. L. Keddie et al. Europhys. Lett. 27, 59 (1994).
[2] T. Miyazaki et al. Phys. Rev. E 69,
061803 (2004).
[3] S. Kawana et al. Phys. Rev. E 63,
21501 (2001).
[4] T. Kanaya et al. Polymer, 44, 3769
(2003).

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JAEA-Review 2011-050)stinu .bra( ytivitcelfeR gol

(a)

0

-1

-2

-3

-4

d-PS/h-PS/d-PS
T=298K
T=403K
0.01

0.02

0.03

0.04

0.05

0.06

-1

Q ( )
190

surface d-PS

188

(b)

)(ssenkcihT

186

212
208
204
200

160
158

middle h-PS
substrate d-PS

156
154
152
300

320

340

360

380

400

Temperature (K)Fig. 1.
(a) Neutron reﬂectivity proﬁles fromdPS/hPS/dPS stacked thin ﬁlms. (b) Temperaturedependence of thickness for each layer.

1-5-12㻙㻌 㻞㻠㻜㻌㻙

JAEA-Review 2011-050

1-5-13A long-range periodic structure in a mixture of D2 O/3-methylpyridine/NaBPh4
induced by solvation eﬀect
Sadakane K., Iguchi N. and Seto H.
Department of Physics, Kyoto University, Kitashirakawa, Sakyo, Kyoto 606-8502
The solvation effect plays an importantrole in various ﬁelds of natural science.
One of the most interesting issues is its inﬂuence on water and organic solvent mixtures. Recently, Onuki and Kitamura theoretically showed that the solvation effectof salt ion induces a long-range periodic
structure in conjunction with a concentration ﬂuctuation of those mixtures. [1]The binary mixture of water and 3methylpyridine (3MP), which shows LCST
type phase separation, is known to havea large salt effect on the phase separation.
Thus, we have investigated the concentration ﬂuctuation and structural formation of
the mixture of D2 O, 3MP and salt at SANSU. In this study, we focused on the effectof sodium tetraphenylborate (NaBPh4 ) because the solvation effect of anions andcations should be very large.
The SANS proﬁle of D2 O/3MP without
salt could be explained by the OrnsteinZernike function, which is generally applied to near-critical binary mixture,
IOZ ( Q) =I0,
1 + ξ 2 Q2

[1] A. Onuki and H. Kitamura, J. Chem.
Phys., 121, 3143 (2004).
[2] K. Sadakane, H. Seto, H. Endo and M.
Shibayama, J. Phys. Soc. Jpn., 76, 113602(2007).

(1)

where ξ is the correlation length and I0 the
forward scattering proportional to the osmotic compressibility.
On the other hand, the SANS proﬁlesfrom D2 O/3MP/NaBPh4 can not be explained by Eq. (1) because a single peak isobserved around Q = 0.1 Å−1 (See Fig. 1).
Thus, we tried to apply the scattering function proposed by Onuki and Kitamura [1],which shows the existence of a long-range
periodic structure induced by solvation effect of salt ion,
IOK ( Q) =where γ is a dimensionless parametercorresponding to the difference of thestrengths of the cation and anion, and λthe Debye screening length. In this expression,√ the peak position Qm is given by
Qm = γ − 1/λ. All the SANS proﬁles of
D2 O/3MP/NaBPh4 can be well explainedby Eq. (2), and the characteristic repeat distance d increase with increasing temperature (See Fig. 1).
This result could be interpreted that thelong-range periodic structure is induced bya cooperation of the solvation effect and theconcentration ﬂuctuation [2].

Fig. 1. SANS proﬁle of D2 O/3MP (the weight fraction of 3MP is 0.32) with 100 mM of NaBPh4 . The
solid line shows the ﬁtting function given by Eq. (2).
The inset shows the temperature dependence of repeat distance, d.

I0,
1 + (1 − γ2 /(1 + λ2 Q2 ))ξ 2 Q2
(2)
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JAEA-Review 2011-050

1-5-14Eﬀect of polymer on uni-lamellar vesicle in lipid mixture system
Norifumi L. YAMADA and Naoya TORIKAIHigh Energy Accelerator Research Organizationin size, and a new Bragg peak due to
MLVs appeared around q = 0.1 Å−1 above
50.0 mg/ml. From these results, we conclude that the addition of PEG stabilize
MLV structure instead of ULV structure.
This would be resulted from the entropic
effect due to the addition of PEG.
References[1] Reeves J. P. and Dowben R. M., J. Cell. Physiol. 73 (1969) 49.
[2] N. L. Yamada et al., Europhys. Lett. 80 (2007)
48002.
[3] M.-P. Nieh et al., Biophys. J. 82 (2002) 2487.
[4] S. Okabe et al., J. Appl. Cryst., 38 (2005) 1035.
10

10

9

10

8

10

7

10

MLV

6

10
I(q) [arb. unit]

It has been well known that natural
swelling of a dry phospholipid ﬁlm usually produces large multi-lamellar vesicles (MLVs) [1]. These mimic biomembranes produced from synthetic phospholipid molecules have been extensively
studied to understand the actual behavior of real biomembranes. Living cells
and their organelle, however, exist as unilamellar vesicles (ULVs). Therefore, effective methods to create the ULVs have beenstudied so far [2].
For a phospholipid mixture system
consisting of long- and short-chain lipids,
ULVs were spontaneously formed athigh temperature when lipid bilayers arecharged by adding ions or charged lipids[3]. Since these ULVs are uniform in sizeand very easy to make, the ULV production
method from bicelles appears promising
to create ideal model cells. In this study,
we investigated the effect of polyethylene
glycol (PEG), as mimic-biomolecules, on
ULV formation in a lipid mixture system.
To observe the ULV structure, wehave performed SANS experiments ona typical lipid mixture system, dimyristoylphosphatidylcholine (DMPC) anddihexanoylphosphatidylcholine (DHPC)
mixture, at SANS-U, JRR-3M, JAEA, Tokai,
Japan [4]. The mixture of lipids in themolar ratio of [DMPC]:[DHPC] = 3.2:1 wasdissolved in the PEG solution to be thesame volume fraction of lipids (0.35 wt.%
for PEG-less sample).
The molecularweight of PEG was 4000 g/mol and theconcentration of PEG solutions were 0,
16.6, 33.3, 50.0, 66.6, 83.3, and 100 mg/ml.
Figure 1 shows the obtained SANS proﬁles of vesicles at high temperature phase(50◦ C). As shown by previous study, homogeneous ULVs were observed in the proﬁle of 0 mg/ml. With increasing PEG
concentration, ULVs became polydisperse

100 mg/ml

5

1083.3 mg/ml

4

1066.6 mg/ml

31050.0 mg/ml

2

1033.3 mg/ml

1

1016.7 mg/ml

0

10

ULV

0 mg/ml

-1

10

-2

10
2
0.001

4 6 8

0.01

2

4 6 8
-1

0.1

2

4 6 8

1

q [Å ]

Fig. 1. SANS proﬁles of vesicles from bicelle withchanging PEG concentration.

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JAEA-Review 2011-050

1-5-15

Studies on Structural Nonuniformity of Natural Rubber
M. Shibayama(A) , T. Suzuki(A), N. Oosaka(A), H. Endo(A), N. Higashitani(B),Y. Morita(B), Y. Kokubo(B), Y. Ikeda(B), and S. Kohjiya(C)(A)ISSP-NSL, Univ. Tokyo, (B)Grad. Sch. Sci. Technol., Kyoto Inst. Tech.,(C)Fac. Sci., Mahidol Univ.
Crosslinked rubbers are one group of the
traditional soft matters. It is well known
that the crosslinked rubber has nonuniformity in its microstructure. However, thisnetwork nonuniformity has not been sufﬁciently elucidated due to the complexity of the composition and the complex
preparatory processes. The goal of thestudy is an elucidation of nonuniformityof crosslinked natural rubber (NR). An upturn scattering was detected in SANS proﬁles of crosslinked and uncrosslinked NR,
which were ascribed to the non-rubbercomponents in NR [1]. Thus, a model research using a synthetic analogue of NR
becomes necessary. In this study, the microscopic structure of peroxide-crosslinked
and sulfur-crosslinked isoprene rubber (abbreviated as P-IR and S-IR, respectively) is
investigated by SANS.
P-IR and S-IR were prepared by millingwith crosslinking reagents and heatpressed for curing at 155 °C and 140 °C, respectively. SANS experiments werecarried out at SANS-U (C1-2), JRR3M in
JAEA (Tokai). The wavelength was 7 .
The sample-to-detector distances were 2.00
and 8.00 m. The scattered intensity wascollected with an area detector and thencircularly averaged. Swollen samples indeuterated (D-) toluene were subjected to
SANS measurements.
The following conclusions were obtained:(i) In both samples, the inhomogeneity
in their network structures was detected,
which was speculated to be due to the presence of poor and rich phases of crosslinking
sites. (ii) The scattering curves of swollen
P-IR and S-IR in D-toluene were successfully reproduced by the Squared-Lorentz
and Lorentz functions. (iii) The mesh size(ξ) and the scale of inhomogeneity as-

cribed to the rich phase (Ξ) in P-IR weredecreased and increased, respectively, by
the increase of network-chain density (ν)
as shown in Fig.1. (iv) For S-IR, ξ was almost constant regardless of the amountsof sulfur and accelerator, whereas Ξ increased with the increase of these amounts
when deﬁnite amounts of stearic acid andZnO were mixed. (v) The increase of ZnO
resulted in the decrease of ξ and Ξ. The
obtained results will be useful for a more
systematic material design of future rubber
products.
Reference[1] T. Karino et al., Biomacromolecules, 8,693(2007).

Fig. 1. Fig.1 ν dependence of ξ and Ξ for P-IR.
The lines are guides for eyes.

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JAEA-Review 2011-050

1-5-16
Temperature Eﬀects on Shear-Induced Structural Transition in the Lamellar Phaseof a Nonionic Surfactant -Change in the Orientation of LamellaeYuriko Kosaka, Makiko Ito, Youhei Kawabata, and Tadashi Kato
Tokyo Metropolitan University
In the past 15 years, much attention
has been paid to the effects of shear ﬂow
on the structure of a lamellar phase owing to the development of the apparatus
which enables us to determine their structures directly under shear ﬂow. In the previous studies, we have measured small
angle neutron scattering (SANS) on thelamellar phases of a nonionic surfactant
C16H33(OC2H4)7OH (C16E7) in D2O at
70C under shear ﬂow with shear rate of
0.01 - 10 s-1. We have found anomalous decrease in the lamellar spacing (d) for the
shear rate of 0.1-1 s-1 [1-3]. In addition,
abrupt change of d has been observed ataround 70C when the temperature is raised
from 60C to 80C. In the present study, we
have investigated effects of temperature in
more detail focusing on the change in theazimuthal intensity distribution.
Measurements of SANS were carried out
at the instrument SANS-U of Institute for
Solid State Physics of University of Tokyo
in JRR-3M at Tokai with a Couette shear cell
[4].
Figure 1a shows azimuthal intensity
distribution for the shear rate of 3 s-1 atdifferent temperatures and at 48 wt% of
C16E7. At 60C, the lamellae is oriented to
the neutral direction (90 and 270 degree)
after the application of shear ﬂow. The
orientation becomes even more strong at
71 C. In Figure 1b, temperature dependences of the peak intensity for the neutral
and ﬂow direnctions are presented. Thisﬁgure demonstrates that the orientation oflamellae becomes abruptly strong at 71 C
and then changes towards isotropci orientation with the further increase in temperature. It should be noted that the repeat
distance also abruptly increases at 71C as
described in the previous report. These results suggest lamellar to onion transition

with increasing temperature, which is notobserved at rest.
References[1] T. Kato et al. Langmuir 20 (2004) 3504.
[2] T. Kato et al. J. Phys. Cond. Matt. 17(2005) S2923.
[3] K. Miyazaki et al. J. Appl. Cryst. 40(2007) s332.
[4] Y. Takahashi et al. J. Soc. Rheol. Jpn. 28(2000) 187.

Fig. 1. Azimuthal intensity distribution at different
temperatures (a) and temperature dependences ofthe peak intensity for the neutral (open diamond)and ﬂow (closed diamond) direnctions (b) at theshear rate of 3 s-1 and at 48 wt% of C16E7.

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JAEA-Review 2011-050

1-5-17

Correlation between local dynamics and gas permeability of substitutedpolyacetylenes by quasielastic neutron scattering
T. Masuda1 , T. Kanaya2 , R. Inoue2 and O. Yamamuro3
1 Department of Polymer Chemistry, Kyoto University, 2 Institute for Chemical Research, Kyoto

University, 3 Institute for Solid State Physics, University of Tokyo

permeability coefﬁcient of O2 . These ﬁndings suggest that slow local motion plays
major role in gas permeability. This tendency is also visible for the permeability
coefﬁcient of O2 dependence of product ofΓ and A for both quasielatic components,
as indicated in Figure 1 (b). The behavior of dynamics of these polymers seemed
to be explained by the model suggested by
Kanaya et al [2]. The detailed analysis is
now under progress.
References [1] K. Tsuchihara et al. Macromolecules, 25, 8548 (1991). [2] T. Kanaya et
al. Macromolecules, 35, 5559 (2002).
0.007

Q=1.64-1
T=300K

0.006(a)observed
fitting curve
narrow component
broad component
flat background0.005)stinu .bra( )w ,Q(Sd function

0.004
0.003
0.002
0.001
0.000

-1

0

1

Energy transfer (meV)

2

3

1

(b)

0.1

G
0.01

A

It is well known that some substitutedpolyacetylenes show high gas permeability
among all the examined polymers [1]. We
synthesized a variety of substituted polyacetylenes [2,3] and investigated the relationship between gas permeability andside-group structure. Through these studies, we observed that local mobility of sidegroup structure in glassy state plays an important role for gas permeability. In order
to conﬁrm this idea, we have investigatedlocal dynamics of several polyaetylene
with bulky substitutes using a quasielastic neutron scattering spectrometer AGNES
installed at the cold neutron guide C3-2-1.
In this study, we mainly focused on thecorrelation between local picosecond dynamics and the gas permeability of thesepolymers. Although glass transition temperatures of investigated polymers are
far above room temperature, investigatedpolymers exhibited quasielatic-like spectrum at room temperature, as shown in Figure.1 (a). It suggests that certain stochastic motion exists even in glassy state. In
order to extract the dynamical feature ofthese polymers, we performed curve ﬁt to
the obtained S(Q, ω). First, we tried to ﬁt
with single Lorentizan function, however
we failed to describe observed spectrumwith single Lorentizan. Hence, we employed two Lorentzian functions and we
could describe the observed spectrum wellwith two Lorentzian functions. We termed
broad quasielatic component and narrowquasielatic component as broad component
and narrow component, respectively. Neither relaxation rate Γ and fraction A of
broad component depend on permeability,
however both Γ and A of narrow component exhibited positive correlation with on

0.001

broad component
narrow component

0.0001
10

-7

-6

3

10

-5

2

PO2(cm (STP)cm/(cm s cm Hg))

10

Fig. 1. (a) An example of ﬁts to S(Q, ω) of one polymer and the quasielastic components were well ﬁtted by two Lorentzians. (b) PO2 dependence of the
product of fraction (A) and relaxation rate of bothquasielastic components.

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JAEA-Review 2011-050

1-5-18
Crowding eﬀect on the shear induced structural transition of lamellar phase
Shuji Fujii(A) and Yohei Kawabata(B)(A) Dept. Material Sci. and Tech., Nagaoka Univ. Tech. (B) Dept. Chem., Tokyo Metropolitan
Univ.
induced Onion formation behavior.

(a)

(b)

(c)
C10E3
C10E3+P105(1%)

I /au.

It is well known that the shear ﬂow applied on a lyotropic lamellar phase induces
an onion (multilamellar vesicle) structure.
Although it is also well known that polymers grafted on the lamellar membrane
affect its dynamics, much less is known
how the grafted polymer chain inﬂuences
the viscoelasticity of lamellar phase, especially how the shear induced lamellar toonion structural transition is inﬂuenced bygrafted polymer chain. On the shear induced lamellar to onion transition for thepolymer-grafted lamellar phase, we should
clarify the bilayer membrane structure in
the microscopic scale.
In the present study, we have measured
the small angle neutron scattering (SANS)
on the polymer-grafted lamellar phasein D2O under shear ﬂow ﬁeld. Samples
used in this study were nonionic surfactant (C10E3)/PEO-PPO-PEO type amphiphilic triblock copolymer (P105)/water
system. Triblock copolymer concentration
was ﬁxed to the mole fraction of 0.01.

0.0

0.5

1.0

1.5

2.0

-1

q /nm

Fig. 1. SANS proﬁles of the surfactant lamellar andpolymer-grafted lamellar phases.

The Rheo-SANS measurements were performed by using SANS-U spectrometerequipped with quartz Couette shear cellat Institute for Solid State Physics, The
University of Tokyo in JRR-3M at Tokai.
Fig.1 shows the SANS proﬁles for surfactant lamellar and polymer-grafted lamellar
phases at shear rate of 50s-1. For the surfactant lamellar phase (ﬁg.1a), SANS proﬁle shows an Onion formation with one
Bragg peak. However, for the polymergrafted lamellar phase (ﬁg.1b), no Onion
formation is observed but SANS proﬁleshows the emergence of the second Bragg
peak, which indicates the lamellar-lamellar
phase separation. Thus, the present results suggest that lamellar-lamellar phaseseparation signiﬁcantly affects the shearActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

1-5-19Nanostructure of Non-Surface Acitive Ionic Amphiphilic Diblock Copolymers in
Aqueous Solutions
Hideki Matsuoka, Hao Chen, Fumiaki Ozaki, Tasuku Yamada
Department of Polymer Chemistry, Kyoto University
I.Introduction”Non-Surface Acitive Amphiphilic Polymer” is a new class of substance which
has been found by our group. It is diblock
copolymer consists of ionoc segment andhydrophilic chain. It shows a very curious
character which has been never observed
for any kind of other molecules: The polymer forms micelles in aqueous solution but
does not adsorbed on the air/water interface. This behavior of out-of-common
sense of surface and interface science andmakes a strong impact on the deﬁnitionof ”Surfactants”, which is a combinationof ”Suraface” ”Active” ”Agent”. The originof this strange behavior should be electrostatic origin since non-ionic polymer nevershows similar behavior. By our systematical investigation, the image charge effect at
the air/water interface is considered to be
an important factor for this phenomenon.
Also, by our study using polymers withvarious chain lengths and length ratios, It
has been found that the degree of polymerization of each segment of, at least, 20
is required to show non-surface active nature. Hence, ”non-surface activity” is somekind of ”Polymer Effect”. In this study, thenanostructure of micelles of non-surface active polymers was investigated by SANS,
and the effect of chain length ratio was duly
examined.
II.Experimental
The polymers used were diblock
copolymers of poly(n-butyl acrylate) andpoly(styrene sulfonate sodium salt) withvarious chain length with keeping constant
block ratio of 1:1. The block copolymers
were synthesized by nitroxy radical mediated living radical polymerization asreported previously. The SANS experiments were carried out with SANS-U

spectrometer of ISSP, University of Tokyo,
at Tokai, Ibaragi, Japan. The measurements
were performed at two different camera
length, i.e., 2m and 8m. The effect of salt
was also investigated with using 0.5M
NaCl aq. as solvent.
III. Results and Discussion
Figure 1 shows SANS proﬁles for solutions of polymers with block ratio, m:n,
=18:13, 28:32, and 37:35. The concentrationof polymer is 0.5 wt.%. A strong scattering was observed for each solution, whichmeans micelle formation in aqueous solution. Although the detailed analysis has
not yet performed since SANS experiments
were carried out only a few weeks ago, thetrends that short chain polymer forms rodlike micelles and long chain polymer forms
mixture of spherical and rod-like micelles.
The blob scattering from micelle coronais also observed. No signiﬁcant difference
is observed SANS proﬁles for no salt and0.5M NaCl conditions, which means very
tough nature of micelle structure against
salt addition.
The SANS proﬁles will be analyzed bycore-shell model and core-corona modelﬁttings to evaluate nanostructural parameters of micelles such as core size,shell thickness, radius of gyration of shellchains, and fraction of spherical and rodlike micelles when coexist. The structuralparameter thus evaluated will be duly examined with single chain properties suchas non-surface activity and cmc (critical micelle concentration). These information will
make a large contribution to correct understanding of ”non-surface active” polymer,
which is a novel class of molecules.

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JAEA-Review 2011-050

Fig. 1. SANS proﬁles of poly(n-butyl acrylate)b-poly(sodium styrenesulfonate) block copolymers
with different block lengths at no and 0.5M NaClconditions.

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JAEA-Review 2011-050

1-5-20

2D-SANS Pattern Observed for Injection Molded Isotactic Polypropylene
T. Sakurai, Y. Nozue, S. Kimata, T. Kasahara, N.Yamaguchi, H. Endo*, M. Shibayama*
Petrochemicals Research Laboratory, Sumitomo Chemical. Co. Ltd. Chiba 299-0295, Japan*Institute for Solid State Physics, The University of Tokyo, Kashiwa 277-8561, Japan
Recently we have successfully demonstrated time-resolved Small-angle neutron scattering (SANS) measurements forobserving melting behavior of injection
molded isotactic polypropylene (iPP) using
deuterium labeling to distinguish different chain lengths within an overall distribution. For SANS pattern with streak andspot shapes in the direction perpendicularand parallel to the ﬂow direction, we clariﬁed that the streak pattern disappeared at
higher temperature compared to the spot
pattern. This result strongly suggests thatthe streak pattern derives from the formation of ”shish” structure in the material andthe spot pattern due to the stacking lamellae structure (”kebab”) [1].
In order to perform the quantitative analysis for shish structure, the SANS data inwider q range is desirable. In this study,
we tried to SANS measurements of injection molded iPP in lower q range.
The deuterated and hydrogenated iPPs
having molecular weight (MW) of ca.
1,200,000, 180,000 and 40,000 with narrow MW distribution were polymerized
by metallocene catalyst system. The ratio of High, Middle and Low MW component in the blend was H:M:L=2:4:1. Total weight of the sample was 7g, and 1gof the sample was deuterated polymer.
Blended samples were selectively deuterated in High or Middle or Low MW component, the deuterated blend samples being called High-D, Mid-D and Low-D. For
the preparation of pseudo-injection sample, compact injection machine developedby co-worker was applied. Detailed preparation method is described elsewhere [1],[2].
SANS measurement was performed at
SANS-U apparatus, at Institute for Solid
State Physics, The University of Tokyo,

Tokai, Japan. The wavelength was 7.0
and the scattered intensity was collectedwith an area detector during 7200 sec. The
sample-to-detector distance was set to be
12 m for lower q measurement, and the experiment was carried out at room temperature.
Fig. 1 shows 2D-SANS data of High-D,
Mid-D and Low-D. As like 2D-SANS pattern observed for camera length of 8m [1],the streak pattern was observed in the direction perpendicular to the ﬂow direction.
The shape of streak pattern depended on
the deuterated MW component, and thedegree of anisotropy was in the order of
Low-D > Mid-D > High-D. The HighD sample showed 2D-SANS pattern withslight anisotropy even in the present camera length.
References[1] S. Kimata et al., Science 316, (2007) 1014.
[2] M. Seki et al., Macromolecules 35, (2002)
2583.

Fig. 1. Figure 1: 12m SANS data in Low-D (left),
Mid-D (center) and High-D (right). Vertical direction is the ﬂow direction.

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1-5-21
Dynamical Properties of Syndiotactic Polystyrene (sPS) Crystalline Complex Phase
Fumitoshi Kaneko, Tatsuya Kawaguchi, Koichi Ute
Graduate School of Science, Osaka University; Graduate School of Engineering, Tokushima
University
Syndiotactic polystyrene (sPS) is a relatively new commodity polymer, which exhibits a variety of solid states. One of theimportant properties of sPS is the formation of crystalline complex phase, whereorganic compounds are stored in the cavities formed between sPS helices with TTGG
conformation. Formerly it was consideredthat only relatively small molecules could
be incorporated into sPS complex phase.
However, recent our studies have clariﬁed that sPS has an ability to form crystalline complexes with larger and bulkier
molecules, exceeding the size limit expected in the previous studies. By using
the help of a plasticizing agent, a wide
variety of molecular compounds can now
be introduced into the crystalline matrix
of sPS. In this study, we have investigated the dynamical properties of suchsPS complex systems containing relatively
large molecules.
We chose several molecules consisting of ethyleneoxide (-CH2CH2O-) groups
as guests. All QNS spectra were measured with AGNES spectrometer of JRR3M(Tokai). The mean-square displacement<uˆ2> of hydrogen atoms was evaluatedfrom the Q dependence of the elastic scattering intensity I(Q) by using the following
the Debye-Waller formula: I(Q)=I(0) exp[(1/3)<uˆ2> Qˆ2], where I(0) is the elastic
intensity at Q=0.
Figure 1 shows the temperature dependence of <uˆ2> for sPS complexes with triethylene glycol dimethyl ether (TEGDM)
and an oligomeric sample (PEG1000). The<uˆ2>s of the two sPS complexes show
similar tendencies to temperature variations, but <uˆ2> is clearly larger insPS/TEGDM than in sPS/PEG at 160 and
230 K. The quasielastic component is also
more intense in sPS/TEGDM. These ex-perimental results indicate that TEMDM ismore mobile than PEG1000 in this temperature region. The temperature dependenceof <uˆ2> can be interpreted as follows.
The molecular motions of both the guest
molecules conﬁned in the cavities are restricted by the host-guest interaction in low
temperatures, but the shorter molecule,
TEMDM, having two mobile methyl terminals starts large diffusive motions fromlower temperatures. For more detailed
analysis, we are planning the experimentto evaluate the contribution of each component (sPS host framework, amorphous region and guest molecules) to QNS.

Fig. 1. Temperature dependence of <u2> for sPS
crystalline complex phase

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JAEA-Review 2011-050

1-5-22
Electrostatic Self-Assembly of Neutral and Polyelectrolyte Block Copolymer andOppositely Charged Surfactant
Masahiko Annaka, Tsuyoshi Matsuda, Kanae Morishita
Department of Chemistry, Kyushu University
dius is ranging between 150-160 A depending on the charge ratio and temperature,and the intermicellar distance of the DTAˆ+
micelles is ˜39 A, which is independent of
the charge ratio Z as well as temperature.
The corona of the complex is constituted
from the thermosensitive PNIPAM. The
aggregation number expressed in terms of
DTA+ micelles per complex is also determined using the analogy with the homopolyelectrolyte/surfactant system, andfound to be 200-250 depending on the
charge ratio and temperature.

(A)

S

CH3
NC C

CH )m ( CH2

( CH2

C O

CH3

CH ) S C
n
COOH

HN
CH
H3C

CH3

0

(B)

102

10

Z = 0.5

Intensity / cm-1

Z = 0.3

101
10-1

100
q0
10-1

10-2

102

q-3/2
10-2

10-1

10-2

10-2
10-1

Z = 0.7

Z = 1.0

q0

q0

101
Intensity / cm-1

Interactions between polyelectrolytes andoppositely charged amphiphiles have attracted a great deal of interest in the last
decades, due to their importance both infundamental polymer physics/biophysics
and in biological and industrial applications. The interactions between polyelectrolytes and oppositely charged surfactants are quite strong and can induce a complex formation, often resulting
in highly ordered structures. These welldeﬁned supramolecular structures of thepolyelectrolyte-surfactant complexes haveunusual properties. We investigate the microscopic structure of colloidal complex
made from poly(N-isopropylacrylamide)block-poly(acrylic acid) (PNIPAM-b-PAA)(Fig. A) as thermosensitive neutral-anionicblock copolymer and dodecyltrimethylammonium bromide (DTAB) as cationic surfactant under various conditions, specifically the effects of the DTAB concentration (surfactant-to-polymer charge ratio
and temperature.
PNIPAM-b-PAA with low polydispersity
was prepared by RAFT polymerization inmethanol. SANS (Fig. B) clearly indicatesthat the aqueous solution of PNIPAM-bPAA and DTAB associate into colloidal
complexes. For low surfactant-to-polymer
charge ratio Z(= [S]/n[P], [S]: DTAB conc.,[P]: PNIPAM-b-PAA conc., n: degree ofpolym. of PAA block) lower than the critical value Zc, the colloidal complexes are
single DTAB micelles dressed by a few
PNIPAM-b-PAA (Fig C-i). Above the critical value Zc ˜ 0.7, the colloidal complexes form a core-shell microstructure(Fig. C-ii). The core of the complex consists of densely packed surfactant micelles(DTA+), and PAA block chains bind tothese micelles, displace their counteranions(Br-) and bridge them together. The core ra-

101

100
10-1

(C)

100
10-1

10-2
10-3

102

10-2
-2

-1

10

10
q / Å-1

10

-2

-1

10

10-3

q / Å-1(ii) ZC < Z(i) Z < ZC
PAA block

~ 39Å
~ 39Å
DTAB micelle
PNIPAM block
coronacore

Fig. 1. (A) Chemical structure of PNIPAM-b-PAA.
(B) SANS proﬁles for 0.4 wt% aqueous solutionsof PNIPAM-b-PAA. (C) Schematic representation ofcomplex (i) Z < ZC, and (ii) ZC < Z.

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JAEA-Review 2011-050

1-5-23
Eﬀects of Molecular Weight and Surface Density on Conformation ofPoly(N-isopropylacrylamide) Brushes Immobilized Onto A Substrate
Masahiko Annaka(1), Yoshihisa Fujii(2), Hironori Atarashi(2), Keiji Tanaka(2),Toshihiko Nagamura(2), Masahiro Hino(3)
1. Department of Chemistry, Kyushu University, Fukuoka 812-8581, Japan.
2. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan.
3. Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan.
In the future, the quantity of polymeric materials used for medical diagnosis and treatment will continue to increase.
Poly(N-isopropylacrylamide) (PNIPAm) is
well known to exhibit LCST-type phase behavior in water. This property has been
cleverly utilized in number of biomedical
application. In such an application, thepolymer surface is in contact with a water phase and polymer is used in various temperatures. Previously, we studiedinterfacial structure of water/poly(methyl
methacrylate), which was a simple model
for water/PNIPAm. As a result, the water/PMMA interface was diffuse in comparison with the air/PMMA one due to theinterfacial roughening and the partial dissolution of segments at the outermost region of the ﬁlm. [1] In addition, the PMMA
ﬁlm was discernibly swollen even in water.
Then, our interest is what happens with theaggregation structure of the PMMA ﬁlm inwater if the temperature increases.
A ﬁlm of perdeuterated PMMA (dPMMA) was prepared from a toluene solution, spin-coated onto a quartz block. The
ﬁlm thickness, evaluated by ellipsometry,was 60.7 nm. The density proﬁle of thedPMMA ﬁlm along the direction normal
to the surface was studied by the multilayer interferometer for neutrons (C3-1-22, MINE) at ISSP, the University of Tokyo.
Prior to the measurement, the dPMMA ﬁlm
was aged in water at 360 K for 12 hr, which
was enough to cause swelling. Incident
neutrons with the wavelength of 0.88 nm
and the resolution of 5.1 % were guided
into the specimen from the quartz side,which was vertically mounted on a goniometer. The reﬂectivity was calculatedon the basis of the scattering length density
proﬁle using Parratt32, which is a freewarefrom the Hahn-Meitner Institute.
Fig. 1(a) shows the scattering vector, q dependence of reﬂectivity for dPMMA ﬁlm inwater. Solid line denote the best-ﬁt calculated reﬂectivity, to the experimental data,on the basis of model scattering length density (b/V) proﬁle in the panel (b). Since thecalculated curve is in good agreement withthe experimental data, it can be claimed
that the model (b/V) proﬁle used well reﬂect the density proﬁle of the dPMMA ﬁlm
along the direction normal to the interface.
The water content in the interior region,
namely constant density region, of the ﬁlm
was 4.0 vol%. Moreover, the overall watercontent of the entire ﬁlm was 9.5 vol%, being much larger than the reported value of
3.4 vol% at room temperature.[1] Since thedPMMA ﬁlm contained water molecules
after being immersed in the water, it became much thicker than before, the thickness increasing from 60.7 to 66.5 nm. The
increment of the ﬁlm thickness was almost
identical to the value calculated on the basis of the overall water content through themass balance. In the case of the ﬁlm aged ina hot water, the most striking feature is thatwater molecules were preferentially segregated at the substrate interface. Taking into
account that the ﬁlm sometimes peels offfrom the substrate during the aging process
in the hot water, this result was quite reasonable. Such an interfacial segregation ofwater was not observed for the ﬁlm aged inwater at room temperature. A more conclusive discussion about an effect of temperature on the aggregation structure of thedPMMA ﬁlm in water will be reported in

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JAEA-Review 2011-050

the future.
Reference[1] K. Tanaka, Y. Fujii, H. Atarashi, M. Hino
and T. Nagamura, Langmuir, 24, (2008) 296.

Fig. 1. (a) Neutron reﬂectivity for a dPMMA ﬁlm inwater. Open symbols depict experimental data, andsolid line is reﬂectivity calculated on the basis of thescattering length density proﬁle shown in (b).

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JAEA-Review 2011-050

1-5-24

Analysis of Adsorption Behavior for Proteins onto (Liquid/Polymer) Interface
Yoshihisa Fujii(1), Hironori Atarashi(1), Keiji Tanaka(1), Toshihiko Nagamura(1),Masahiro Hino(2)
1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan
2. Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
Recently, polymer ﬁlms have been widelyused in a wide variety of applications. In
biomaterials and biosensors, the polymer
surface is in contact with a water phase.
Thus far, a density proﬁle of a perdeuterated poly(methyl methacrylate) (dPMMA)
ﬁlm spin-coated on a substrate was examined in water along the direction normal tothe interface by specular neutron reﬂectivity (NR).[1] The interface of dPMMA withthe water was much more diffused than thepristine air/dPMMA interface. This was
because segments at the outermost regionof the ﬁlm could be dissolved into the water phase. If the length of the segments
can be controlled, adsorption behaviors oflipids and protein even onto PMMA in water might be controlled. Since the former
will be realized by the technique of a precise synthesis in the near future, adsorption
behavior of protein onto a PMMA ﬁlm wasstudied as a ﬁrst benchmark.
A ﬁlm of dPMMA was prepared from atoluene solution, spin-coated onto a quartz
block. The ﬁlm thickness, evaluated byellipsometry, was 60.4 nm. As protein
and buffer solution, bovine serum albumin(BSA) and 0.1 mol/l phosphate buffer solution were used, respectively. The density
proﬁle of the dPMMA ﬁlm along the direction normal to the surface was examined by
the multilayer interferometer for neutrons(C3-1-2-2, MINE) at ISSP, the University ofTokyo. Incident neutrons with the wavelength of 0.88 nm and the resolution of 5.1% were guided into the specimen from thequartz side, which was vertically mounted
on a goniometer. The reﬂectivity was calculated on the basis of the scattering lengthdensity proﬁle using Parratt32, which is afreeware from the Hahn-Meitner Institute.
Fig. 1(a) shows the scattering vector, q de-pendence of reﬂectivity for a dPMMA ﬁlm.
For clarity, each data set for the dPMMA
ﬁlm in buffer and BSA buffer solution is
off-set by a decade. Since just one ﬁlm wasused for all measurements, the NR curves
can be directly compared. Solid and broken lines denote the best-ﬁt calculated reﬂectivity, to the experimental data, on thebasis of model scattering length density(b/V) proﬁles in the panel (b). The (b/V)
values for quartz, dPMMA, buffer and BSA
were 3.48x10-4, 6.62x10-4, -5.44x10-5 and2.40x10-6 nm-2, respectively. Since the calculated curves are in good agreement withthe experimental data, it can be claimed
that the model (b/V) proﬁles used well reﬂect the density proﬁles of the dPMMA
ﬁlm along the direction normal to the interface. In buffer, the model (b/V) proﬁle was almost the same as the one inwater reported before.[1] And, as shownin the (b/V) proﬁle, segments at the outermost region of the ﬁlm were dissolved
into the buffer phase. The interface of dPMMA with the BSA buffer solution becamerougher than the one with buffer solution
because of increasing interfacial roughness
via the adsorption of BSA. This roughening was asymmetric to the interface; only
the solution side became rougher. This interfacial roughening after the BSA adsorption was in excellent accord with the direct
observation for the interface using atomic
force microscopy. More conclusive study
will be reported in the near future.
Reference[1] K. Tanaka, Y. Fujii, H. Atarashi, M. Hino
and T. Nagamura, Langmuir, 24, (2008) 296.

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Fig. 1. (a) Neutron reﬂectivity for a dPMMA ﬁlm in
air, buffer and BSA buffer solution. Open symbols
depict experimental data, and solid lines are reﬂectivity calculated on the basis of the scattering lengthdensity proﬁles shown in (b).

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JAEA-Review 2011-050

1-5-25Lamellar to Micelle Transition of Nonionic Surfactant Assemblies Induced byAddition of Colloidal Particles
Y. Suganuma, N. Urakami*, R. Mawatari, S. Komura**, K. Nakaya-Yaegashi, M. Imai
Ochanomizu University, *Yamaguchi University, ** Tokyo Metropolitan University
We have investigated the depletion interaction between lamellar membranes andspherical colloidal particles using a small
angle neutron scattering (SANS) technique.
By adding colloidal particles into lamellar
membrane slits, the ﬁrst lamellar peaks in
SANS proﬁles become intense and the second and higher harmonics begin to appear,
indicating that the membrane ﬂuctuations
are suppressed by the colloidal particles.
We estimate the inter-lamellar interaction
potential in the presence of the colloidal
particles from the layer compressibility obtained by the SANS proﬁle analysis andpropose a phenomenological free energy
model based on the restriction of membrane ﬂuctuations. Further addition of thecolloidal particles brings a lamellar membrane to ﬂexible rod-like micelle transition.
In order to release the strong frustration
due to the restriction of membrane ﬂuctuations, the surfactant assemblies transformthe morphology from the two dimensional
sheets to the one dimensional rods. We estimate free energies of the lamellar membrane + colloidal particle mixture and therod-like micelle + colloidal particle mixture
to explain the observed lamellar to micelletransition.

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1-5-26
Nano-meter-sized domain formation in lipid membranes observed by small angle
neutron scattering
Sakuma Y., Imai M., Masui T., *Urakami N.
Ochanomizu University, *Yamaguchi University
Using a contrast matching techniqueof small angle neutron scattering (SANS)
and small unilamellar vesicles (SUVs) composed of ternary mixture of deuteratedsaturated (d-DPPC), unsaturated (DOPC)
phosphatidylcholine lipids and cholesterol
we have investigated macroscopic liquiddisordered and liquid-ordered phase coexistence on model biomembranes but theequilibrium size of these domains is constrained to less than 10 nm by the system size. Above a miscibility temperature the ternary vesicles with the matching composition show no signiﬁcant scattering, which represents that the lipids are
mixed homogeneously. However below
the miscibility temperature, a characteristic scattering proﬁle with a maximum isobserved, indicating the formation of domains on SUVs. The observed proﬁles arewell described by a multi-domain model.
In order to explain the obtained results, wehave performed a molecular dynamics simulation with a coarse grained model. Bothexperimental and simulation results showthat the domains on the SUVs are agitatedby thermal ﬂuctuations and repeat coalescence and rupture even below the miscibility temperature. These domains are stabilized by decreasing temperature and forma mono-domain.
In addition based on
the SANS data and phase diagram of theternary system we determine the compositions of the domain and the matrix regions,i.e. tie-lines in the phase diagram, whichshows that d-DPPC molecules concentratein the domain region with decreasing temperature.

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1-5-27

Sol-Gel Transition of Hydrophobically Modiﬁed Polyrotaxane
Takeshi Karino, Yasushi Okumura, Changming Zhao, Masatoshi Kidowaki, Toshiyuki
Kataoka, Kohzo Ito, and Mitsuhiro Shibayama
Institute for Solid State Physics, The University of Tokyo, Graduate School of Frontier Sciences,
The University of Tokyo
Recently, we succeeded in preparation ofwater-soluble polyrotaxanes by introducing hydrophobic groups. In the case of
methyl group substitution, i.e., methylated
polyrotaxane (Me-PR), Me-PR aqueous solutions exhibited thermosensitivity and underwent a sol-gel transition by increasing
temperature. The introduction of methylgroups to PRs leads to thermosensitivity. It
is noted here that substitution with largerhydrophobic functional groups, such as
ethyl groups and propyl groups, resulted
in a macrophase separation even at ambient temperature.
In this report, the sol-gel transition andthermosensitivity of Me-PR aqueous solutions were investigated by means of smallangle neutron scattering (SANS) and dynamic light scattering (DLS). It is known
that water-solubility of polyrotaxane (PR),consisting of poly(ethylene glycol) (PEG)
and R-cyclodextrin (R-CD), is very low due
to stacking of neighboring R-CD molecules
on a PEG chain. Methylation of the hydroxyl groups on R-CD molecules resulted
in a signiﬁcant improvement of watersolubility, and Me-PR exhibited a thermoreversible sol-gel transition in water depending on the degree of methylation. For
low degrees of methylation (<30%), a MePR solution was transparent even up to 80°C. On the other hand, for high degrees
of methylation (>60%), it became opaquewith increasing temperature and a gelation
took place at high temperature. The temperature dependence of the sliding motionof CD molecules along the PEG chains andthe mechanism of sol-gel transition are discussed on the basis of SANS and DLS results.

[1] Y. Okumura and K. Ito, Adv. Mater. 13,
485 (2001).
[2] T. Kataoka, M. Kidowak, C. Zhao, H.
Minamikawa, T. Shimizu and K. Ito, J.
Phys. Chem., B, 110, 24377 (2006).
[3] T. Karino, Y. Okumura, C. Zhao,
M. Kidowaki, T. Kataoka, K, Ito and
M. Shibayama, Macromolecules, 39, 9435
(2007).

References
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1-5-28Structural Study on Uniaxial Extension of Nanocomposite Hydrogel with HighClay Concentration by Means of Contrast Variation Neutron Scattering
T.Nishida1 , H. Endo1 ,N. Osaka1 , K. Haraguchi2 M. Shibayama1
Institute for Solid State Physics, The University of Tokyo, Kashiwanoha 5-1-5, Kashiwa, Chiba
277-8581, Japan1 , Kawamura Institute of Chemical Research, 631 Sakada, Sakura-shi, Chiba
285-0078, Japan2
In these days, mechanically excellent
gels are developed such as topological gels,double network gels, and nanocomposite
gels (NC gels). NC gels are hybrid materials consisting of organic polymers (poly(Nisopropyl acrylamide)) and inorganic clay
nanoparticles (hectorite) , which have excellent physical properties, such as toughness, high modulus, deformability, etc. It
is interesting and important to account forthese mechanical properties on the molecular level for material science as well as
industrial applications. In order to elucidate the microscopic structure of NC gels
under elongation, we carried out contrast
variation SANS (CV-SANS) experiments
by varying the D2 O fraction in the aqueous solvent. Since NC gels are ternary systems consisting of clays, polymers, and water, observation of partial scattering functions reﬂecting each component is straightforward for quantitative structural analyses of the multicomponent system. So the
CV-SANS techniques are essential for oursystem. NC gels are synthesized by polymerization with a mixture of N-isopropyl
acrylamide monomers and Laponite clay
nanoparticles in aqueous solutions. To apply CV-SANS techniques, we prepared ﬁve
different NC gels consisting of 0, 22.6, 70,
80 and 100vol% D2 O fraction. SANS experiments were performed at SANS-U diffractometer of Institute for Solid State Physics,
the University of Tokyo. This experimenthas been the ﬁrst attempt to apply the CVSANS techniques to uniaxially-stretchedhydrogels. With CV-SANS anisotropic 2dimentional SANS patterns were clearlyobserved (see Fig. 1). The stretching ratiois λ = 1, 3, 7. The upper 6 ﬁgures indicate
scattering from clays, i.e., the scattering

contrast between polymer and solvent wasmatched, and bottom 6 ones are from polymers, i.e., the scattering contrast between
clay and solvent was matched. The highQ (detector length=2m) 2-dimensional patterns show elliptic pattern reﬂecting thesimilar orientations of clay and polymer for
the uniaxial stretch. The low-Q (detector
length=8m) patterns show similar two-lobe
patterns for both clay and polymer scattering at λ = 3, which differ at λ = 7.
This tendency clearly indicates that polymers are adhered to clay surfaces, whichstart to be torn off at λ = 7. Reference
S. Miyazaki et al., Macromolecules 39, 8112,(2006).

Fig. 1. 2-dimentional SANS patterns for uniaxially
stretched NC gels at high-Q and low-Q.

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6 Biology

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1-6-1

Control of Membrane Lipid dynamics by Transmembrane and Amphipathic
PeptidesM. Nakano(A), M. Fukuda(A), T. Kudo(A), H. Endo(B)(A)Graduate School of Pharmaceutical Sciences, Kyoto Univ., (B)ISSP-NSL, Univ. of Tokyo
Controlled lipid trafﬁc in biological membranes is important for cell growth, development and survival [1]. For example,
phospholipids that are produced in the cytosolic leaﬂet of the endoplasmic reticulum (ER) membrane can ﬂip to the otherside, which is required to ensure balanced
growth of the bilayer. Although this transbilayer movement of lipids is considered
protein-mediated, it is unclear whether it
involves a dedicated ﬂippase or the mere
presence of proteins in the ER bilayer.
Kol et al. have observed that peptides
that mimic the alpha-helices of transmembrane proteins can stimulate ﬂip-ﬂop of
ﬂuorescence-labeled phospholipids in liposomes [2], which indicates that the ability
to catalyse ﬂip-ﬂop in the ER is not necessarily restricted to one speciﬁc protein.
We recently succeeded in determining
the rates of interbilayer exchange and ﬂipﬂop of dimyristoylphosphatidylcholine(DMPC) in large unilamellar vesicles(LUVs) by small-angle neutron scattering (SANS) technique [3]. In this study,
similar experiments were carried out withlonger acyl chain lipid, 1-palmitoyl-2oleoylphosphatidylcholine (POPC) and its
analogue with smaller polar headgroup,
1-palmitoyl-2-oleoylphosphatidic
acid(POPA), and the effect of the transmembrane peptide on the transbilayer transfersof lipids was investigated.
POPC, POPA, d31-POPC, and d31POPA were obtained from Avanti Polar Lipids Inc. (Alabaster, AL). Transmembrane peptide, KALP23, was obtained from Hayashi Kasei Co. (Osaka).
Methyl-beta-cyclodextrin (MCD) was from
Aldrich (Milwaukee, WI). LUVs consistingof deuterated (D-LUV) or hydrogenatedlipids (H-LUV) with a diameter of ca. 100
nm were prepared by extrusion method

using Tris-buffered saline (10mM Tris-Hcl,
150 mM NaCl, pH 7.4) prepared from mixtures of D2O and H2O. LUVs consistingof 1:1 mixture of deuterated and hydrogenated lipids (D/H-LUV) were also prepared. Transmembrane peptide (if necessary) was mixed (0.5 mol%) with lipids before hydration. Volume fraction of D2O
in the Tris-buffer was 0.3, which corresponds to the contrast-matching condition
between D/H-LUV and solvent. Phospholipid concentration of each LUV preparation was set to 30 mM. SANS measurements were performed at 37 °C using
SANS-U with 7 angstrom of incident neutron beam. Sample-to-detector distance
was set to 4 m.
TR-SANS measurement was started immediately after mixing equivalent volumeof D-LUV and H-LUV. Time-course of thenormalized contrast was calculated fromthe scattering intensity and plotted in Figure 1. POPC showed extremely slow interbilayer exchange with the half-life of
exchange of more than 90 h. Moreover,
POPA, which has smaller polar headgroupthan POPC, showed no exchange. Addition of MCD, which is known to catalyze the interbilayer lipid migration, indeed enhanced the rate of exchange. In thepresence of MCD, the normalized contrast
for POPC LUVs reached to 0.56 and became constant, which suggests that POPC
does not ﬂip-ﬂop at all. Deviation of theconstant value (0.56) from 0.5 is presumably due to the existence of multilamellar
species in LUV preparation. On the other
hand, the contrast decay of POPA LUVs
reached well below 0.5, suggesting an involvement of ﬂip-ﬂop.
We performed the TR-SANS experiments
on LUVs with peptide, KALP23. However,no stimulating effect of the peptide on the

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ﬂip-ﬂop of POPC and POPA was observed.
This result suggests that a mere insertionof transmembrane helices into bilayer does
not mediate the lipid ﬂip-ﬂop.
References[1] J. C. M. Holthuis and T. P. Levine, Nat.
Rev. Mol. Cell Biol. 6 (2005) 209.
[2] M. A. Kol, A. N. C. van Laak, D. T. S.
Rijkers, J. A. Killian, A. I. P. M. de Kroon, B.
de Kruijff, Biochemistry 42 (2003) 231.
[3] M. Nakano, M. Fukuda, T. Kudo, H.
Endo, T. Handa, Phys. Rev. Lett. 98 (2007)
238101.

Fig. 1. Contrast decays of POPC (squares) and
POPA (circles) LUVs after mixing D- and H-LUV at
37 °C in the absence (open symbols) and presence(closed symbols) of 1mM MCD.

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1-6-2
Dynamics of folded and partial unfolded proteins observed by solution inelastic
neutron scattering
H. Nakagawa A , Y. JotiB , O. YamamuroB , I. TsukushiC , M. Kataoka A,D
A JAEA, B Univ. Tokyo, C Chiba Inst. Tech., D NAIST
Protein has biological function under thephysiological condition, which is usuallyin a solution. So far most inelastic neutron scattering experiments with biological samples are limited in the hydrated
powder condition due to the strong solvent scattering. But recently solution inelastic neutron scattering experiments haveemerged in the literature, which is evennow challenging work [1].
We performed solution scattering experiment with AGNES using Staphylococcal
nuclease (SNase) of native and truncatedmutant. The energy resolution of ANGNES
is 120 μeV. Truncated mutant is SNase
without C-terminal 13 residues, which is in
the partial unfolded state under the physiological condition.
Figures are the scattering proﬁles of two
samples at 280 K and 300 K. Under the temperatures the native SNase is in the folded
state. Elastic incoherent structure factor(EISF) of the folded state hardly decreases
upon heating from 280 K to 300 K. This
indicates that the folded structure is thermally stable in these temperatures. On theother hand, EISF of the partial unfolded
state notably decreases upon the heating.
The difference of EISF between two temperatures suggests that conformational entropy of the unfolded protein at 300 K issigniﬁcantly larger than that at 280 K.
The quantitative analysis of solution inelastic neutron scattering will make it possible to characterize the dynamical properties of protein structure and give important
insight into the protein folding problem.

Fig. 1. Solution inelastic neutron scattering spectraof SNase in folded and partial-unfolded states.

[1] J. Fitter et al. : Chem.Phys. , 292, 405(2003).

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1-6-3
Hydration water dynamics at protein dynamical transition by quasi-elastic neutron
scattering
H.Nakagawa(A), Y.Joti(B), O.Yamamuro(C), M.Kataoka(A,D)(A)JAEA, (B)Univ.Tokyo, (C)ISSP-NSL Univ. Tokyo, (D)NAISTA protein dynamical transition around180˜240 K has been observed for the hydrated protein [1]. It was reported for various proteins that their functions are suppressed with the loss of anharmonic dynamics by dehydration or by cooling down
below the transition temperature. In order to elucidate the role of water at theprotein-water interface, it is essential to understand protein dynamics and function
properly. In this study the hydration water
dynamics were examined by quasi-elastic
neutron scattering below and above thedynamical transition temperature at a hydration level of 0.39 (g D2O/g protein).
The scattering from the hydration wateron the protein can be selectively estimatedby the subtraction of the scattering proﬁle of a D2O-hydrated protein from thatof a H2O-hydrated protein. The neutron
inelastic scattering experiments were performed with AGNES, in the JRR-3M reactor in Tokai, which has an energy resolution of 120 μ eV. Figure (a) shows themean-square displacements (MSD) of protein and hydration water at various temperatures. Below the dynamical transition
temperature ˜240 K, the MSD of the protein and the hydration water are almost
identical, while above the transition temperatures the MSD of the hydration water are signiﬁcantly larger than those of theprotein. Figure (b) shows that the inelastic
spectrum of the hydration water is almost
identical to the resolution function at 100 K
and Figure (c) shows that quasi-elastic scattering of the hydration water was observed
at 300 K. These results indicate that above
the dynamical transition temperatures thehydration water has the diffusive motions.
It was reported that a relaxation time ofthe protein-water hydrogen bond network
is 18 ps at 300 K [2]. The observed hydra-tion water dynamics involves such a network relaxation. The dynamical coupling
between hydration water and protein is essential for the protein dynamical transition.
1) W.Doster et al.: Nature ,337,754(1989).
2) M.Tarek et al.: Phys.Rev.Lett ,88(2002).

Fig. 1. Figure Mean-square displacement of protein
and hydration water (a), inelastic neutron scatteringof protein, hydration water and resolution function
at 100K (b) and 300K (c).

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1-6-4
Strctural torlance of complex of αA-crystallin and αB-crystallin
M. Sugiyama1 , N. Fuji1 , Y. Morimoto1 , T. Sato2 ,1 Research Reactor Institute, Kyoto Univ., Osaka, 590-0494

complex has tolerance against UV irradiation even though it includes αB-crystallin.
Therefore, we can conclude that the role of
αA-crystallin in the complex is to preventfrom making abnormal aggregation against
UV irradiation.

Intensity / a.u.

(a) 0.1(a)with UV

0.01

1E-3

1E-4
0.01

(b)

0.1

Intensity / a.u.

Alpha-crystallin is one of chaperones toprevent from abnormal aggregation of proteins in human eye lens. This protein is awater-soluble aggregate consisting of two
kinds of polypeptide, αA-crystallin and αBcrystallin. These two polypeptide have
similar aging acid sequences. Here, it leads
a simple question, why does α-crystallin need
two similar polypeptides?
In order to answer this question, we have investigatedstructural responses of αA-crystallin and
αB-crystallin under environmental stresses,
such as low temperature, UV irradiation,
γ-ray irradiation and so on. By our previous studies, it has been revealed that αAcrystallin and αB-crystallin show different
structural responses against low temperature and UV irradiation: αA-crystallin has
higher structural stability against UV irradiation but lower one against low temperature whereas αB-crystallin shows opposite structural stability against two stresses.
We supposed that by consisting of two
polypeptide which have opposite stability
against low temperature and UV irradiation, α-crystallin could develop tolerance totwo external stress.
In order to prove this hypothesis, weshould reveal the structural response of
the complex consisting of αA-crystallin and
αB-crystallin under the external stresses.
For this purpose, we observed the structural evolution of the complex of αAcrystallin and αB-crystallin under UV irradiation with small-angle neutron scattering. The UV light had wavelength range
with 280-360 nm (UV-B) and the SANS intensity was recorded every 30 minutes for8 hours.
Figure 1(a) shows the SANS proﬁles of
the complex before and after 8 hr UV irradiation at 37 C and Fig. 1(b) also shows thoseat 37C for 0 and 8 hr without UV irradiation. This result clearly indicates that the

before UV
after UV(@37°C, 8hrs)-1

Scattering vector / Åwithout UV

0.01

1E-3

1E-4
0.01

before UV
at 37°C for 8hrs

-1

Scattering vector / ÅFig. 1. SANS proﬁles of the complex αA-crystallin
and αB-crystallin.

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1-6-5

Measurements of slow dynamics of actin
Satoru Fujiwara, Fumiko Matsumoto, Hiroshi Nakagawa, Nobuaki Takahashi, and*Toshiro Oda
Japan Atomic Energy Agency and *RIKEN SPring8-centerF-actin, a helical polymer formed bypolymerization of the monomers (G-actin),plays crucial roles in various aspects ofcell motility. Flexibility of F-actin has beensuggested to be important for such avariety of functions. Understanding the
ﬂexibility of F-actin requires characterization of a hierarchy of dynamical properties, from internal dynamics of theactin monomers through domain motions
within the monomers and relative motions
between the monomers within F-actin tolarge-scale motions of F-actin as a whole.
As one of the ongoing projects towards
this ultimate goal, we have been studying
the dynamics of actin in a pico- to nanosecond time range by neutron spin-echo(NSE) spectroscopy.
As a continuation to the experiments donein 2006, we carried out two kinds of the
NSE measurements: one was the measurements with a wider Q-range in order toobtain the detailed Q-dependency of therelaxation times, from which informationon the collective motions such as the actin
protomers in F-actin and the domain motions in the actin protomer were obtained;
the other was the measurements on longer
time scales, in order to make more accurate
estimation of the relaxation times possible.
G-actin and F-actin were puriﬁed fromrabbit skeletal muscles, and suspended in
D2O. The NSE measurements on these solutions were carried out on the spectrometer iNSE, run by the University of Tokyo,
installed at the guide hall of the research
reactor, JRR-3M, Ibaraki, Japan. Two experimental set-ups enabled us to measure theintermediate scattering functions in the Qrange between 0.04 Aˆ-1 and 0.2 Aˆ-1 at
the Fourier time up to 15 nsec, and thosein the Q-range between 0.03 Aˆ-1 and 0.12
Aˆ-1 at the Fourier time at least up to 30

nsec. Figure 1 shows the combined resultsof these two measurements. It is shownthat although the relaxation times of theintermediate scattering functions of F-actin
is very slow compared to those of G-actin,
each intermediate function can be ﬁt witha single exponential, from which effective
diffusion coefﬁcients can be estimated. Behavior of the effective diffusion coefﬁcientsof G-actin as a function of Qˆ2 corresponds
to free diffusion in solution whereas that of
F-actin seems to reﬂect the collective motions within F-actin. Detailed analysis iscurrently underway.

Fig. 1. The normalized intermediate scattering functions of (a) G-actin and (b) F-actin

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1-6-6Structure and dynamics of β-lactoglobulin aggregates by small-angle neutron
scattering and neutron spin echo methods
K. Yoshida1 , T. Yamaguchi1 , H. Endo2 , M. Shibayama2
1 Department of Chemistry, Faculty of Science, Fukuoka University,2 Institute for Solid State

Physics, The University of Tokyo
Many proteins aggregate and gelate
when they take a misfolded state. The gelation of β-lactoglobulin(BLG) is triggeredby heat, pressure, and addition of alcohol. The pH dependence of the aggregation
state of a heat-induced gel has been studied[1], however, the mechanism of alcoholinduced gelation is not clear. Understanding the mechanism of aggregation of denatured BLG would provide a hint to reveal how misfolded protein forms an aggregate such as amyloid ﬁbril. Small-angle
neutron scattering and neutron spin echomeasurements provide useful informationof the structure and dynamics of the BLG
aggregates.
BLG was lyophilized from D2 O solution to substitute exchangeable hydrogenof BLG to deuterium. The BLG powder was dissolved into ethanol- andtriﬂuoroethanol(TFE)-water mixtures atvarious volume fractions of alcohol andfollowed by addition of 100 mM of DCl
and the BLG concentrations were 10 and
20 mg ml−1 . A sample was kept in aquartz cell of 2-mm path length for SANS
measurement. The cell was inserted into atemperature-controlled chamber at 298 K.
The distances between the sample and detector were 1 and 4 m, corresponding to Q
of 0.007 - 0.3 Å−1 . Measurements were also
made for background and lupolen used forintensity normalization. A quartz cell of
4-mm path length for NSE measurement.
The scattering vector Q covered was 0.055- 0.12 Å−1 . The Fourier time was varied
from 0.15 to 15 ns. The temperature ofsample was controlled at 298 ± 0.3 K withcirculated water.
Figure 1 shows the SANS intensity of
BLG in ethanol-water mixture. This in-dicates that BLG exists as a monomer up
to 20 vol% of ethanol and the aggregation occurs above 30 vol% where the secondary structure BLG changes. A similar
trend was also found in TFE-water mixture. The alcohol-induced BLG aggregation could be well related to the secondary
structure change. The relaxation of BLG
obtained from NSE intermediate scatteringfunctions retards drastically by addition of
ethanol and TFE. The relaxation was hardly
found at an energy resolution of the NSE
spectrometer at 30 vol% of ethanol and 20
vol% of TFE where the solutions gelate, indicating the formation of a rigid BLG network structure.
The present results will be comparedwith those of heat- and pressure-induced
aggregation of BLG. We will discuss therole of solvent on gelation of BLG at themolecular level.
References[1] S. Takata, T. Norisuye, N. Tanaka,
M. Shibayama, Macromolecules 33, 54705475 (2000).

Fig. 1. SANS intensity curves of BLG at various
volume fraction of ethanol in ethanol-water mixture
with 100 mM DCl.

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1-6-7
Neutron Diﬀraction Study of HIV-1 Protease in Complex with Inhibitor
KNI-272
M. Adachi1 , T. Ohhara1 , K. Kurihara1 , T. Tamada1 , E. Honjo1 , N. Okazaki1 , S. Arai1 ,Y. Shoyama1 , H. Matsumura2,3 , H. Adachi2,3 , K. Takano2,3 , Y. Mori2,3 , K. Hidaka4 ,T. Kimura4 , Y. Hayashi4 , Y. Kiso4 and R. Kuroki4
1

2

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki, 319-1195
Graduate School of Engineering, Osaka University, Suita, Osaka 565-0871
3
SOSHO Inc., Osaka 541-0053
4
Kyoto Pharmaceutical University, Kyoto, Kyoto 607-8412

The HIV-1 protease (EC 3.4.23.16) is an
aspartic protease that functions to cleave thenascent viral polyprotein and plays an essential role in viral replication. Currently,
the development of HIV-1 protease inhibitors
is regarded as a major success of structurebased drug design, and the inhibitors of HIV
protease are important compounds to establish highly active antiretroviral therapy for
AIDS. The investigation of catalytic mechanism of HIV-1 protease will help to improvethe design of inhibitor against HIV-1 protease. Thus, in order to identify the locationof key hydrogen atoms, we aimed to determine the structure of HIV-1 protease with its
transition state analog, KNI-272 by neutron
crystallography.
For neutron crystallography of protein, a large
crystal in size is required for data collection. We prepared 1.4 mm3 HIV-1 protease
crystal in volume by two-liquid system andmacro seeding method using the recombinant
HIV-1 protease which is refolded and puriﬁed from Eschericha coli cells. The crystal was soaked into deuterated solution andmounted at BIX-4 of the neutron diﬀractometer at JAEA. Diﬀraction data were collected
at room temperature using a monochromatic
neutron beam (λ= 2.6 Å) and recorded on aneutron imaging plate. For the eﬃcient datacollection, a- and c-axes of the crystal lattice
was leaned at about 45 degree angle relative
to phi rotation axis. A total rotation range of
50.7 was covered by 169 images with an exposure time of 6h/image by rotation angle of 0.3
from a rotation about one independent axis.
The data were processed with the programs
原子炉：JRR-3

装置：BIX-4(1G-B)

DENZO and SCALEPACK. Whole data set
was integrated and scaled to 2.3 Å. Data collection and reﬁnement statistics are summarized in Table 1. Moreover, same crystal wasused to obtain X-ray diﬀraction data to 1.4
Åresolution. From the crystallographic reﬁnement using both x-ray and neutron diﬀraction
data by a joint reﬁnement program PHENIX,
the structure has been reﬁned to R-factor of
16.0 %.

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JAEA-Review 2011-050

1-6-8
Neutron Diﬀraction Study of ADP-ribose pyrophosphatase
M. Adachi1 , K. Kurihara1 , T. Tamada1 , T. Ooga2 , S. Kuramitsu2 and R. Kuroki4
2

1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki, 319-1195
Graduate School of Science, Osaka University, Toyonaka, Osaka 563-0043

ADP ribose pyrophosphatase (ADPRase)
catalyzes the hydrolysis of ADP ribose toribose 5 phosphate and AMP. The postulated role of ADPRase is to control the cellular concentration of toxic nucleoside diphosphate derivatives or physiological methabolites. Yoshiba et al1) reported x-ray crystal structures of ADPRase derived from an
extreme thermophile [Thermus thermophilus] and proposed the catalytic mechanism including ionization state of catalytic residues
and role of water molecules for the catalytic
function and substrate recognition of ADPRase. However, hydrogen atoms of the enzyme, substrate and water molecules have notbeen detected directly because of lower scattering length of hydrogen atom by X-ray compared to other atoms. It is necessary to obtain information of hydrogen atoms by neutron crystallography for understanding thecatalytic mechanism in detail. For neutron
crystallography of a protein, large crystal insize is required for data collection. We prepared 8 mm3 ADPRase crystal in volume
by macro seeding method using recombinant
ADPRase puriﬁed from Eschericha coli cells.
The crystal growth experiment was performed
using PEG4000 as a precipitant and it took
about two months at 20 degrees to obtain
the appropriate size of crystal. The crystal was soaked into deuterated solution andmounted at BIX-3 of the neutron diﬀractometer at JAEA. Diﬀraction data were collected
at room temperature using a monochromatic
neutron beam (λ= 2.9 Å) and recorded ona neutron imaging plate. Although c-axis of
the crystal lattice is rather too long (119Å)for data collection in BIX-3, some diﬀraction peaks were overlapped. After the separation of diﬀraction peaks and completenesswere predicted, full data set was collectedalong two independent axes. A total rota原子炉：JRR-3

装置：BIX-4(1G-B)

tion range of 103.8 degrees was covered by
346 images with a rotation angle of 0.3 degree, and the exposure time was 4h/image.
The data were processed with the programs
DENZO and SCALEPACK. Whole data set
was integrated and scaled to 2.1 Å. Data collection and current reﬁnement statistics are
summarized in Table 1. From the crystallographic reﬁnement using both x-ray and neutron diﬀraction data by a joint reﬁnement program PHENIX, the structure has been reﬁned
to R-factor of 17.4 %.

References
1) Yoshiba S, Ooga T, Nakagawa N, Shibata T, Inoue Y, Yokoyama S, Kuramitsu S, Masui R. J.
Biol. Chem. 279, 163-174 (2004).

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JAEA-Review 2011-050

1-6-9
Trial Diﬀraction Measurements of Protein Single Crystals in H2 O
S. Fujiwara, K. Kurihara and T. Chatake1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494

Among various methods for structural
studies of biological macromolecules, neutron
scattering and diﬀraction provide unique information that cannot be obtained from othermethods. Because of a large diﬀerence in the
scattering length density of water and heavy
water (-0.00562 × 10−12 cm Å−3 for H2 O
and 0.064 × 10−12 cm Å−3 for 2 H(=D)2 O)
due to the diﬀerence in the scattering lengthof hydrogen (-0.3742 × 10−12 cm) and deuterium (0.6671 × 10−12 cm), it is possible tovary widely the scattering length density ofsolvent by changing the fraction of D2 O in
the solvent. This ”contrast variation” technique has found wide applications not onlyin small-angle neutron scattering but also
in neutron crystallography. Application of
the contrast variation technique in neutron
crystallography provides information on individual components in a very large macromolecular complex such as nucleic acid regions within viruses and nucleosomes, and on
disordered components in the complex suchas detergent moiety in membrane proteins1) .
Essence in these applications is obtaining
structural information of the region having
distinct scattering length density. Thus, there
is a possibility that the scattering density ofamino acids is estimated because each aminoacid has distinct scattering length density.
Furthermore, we have obtained the resultsfrom the neutron ﬁber diﬀraction measurements using the contrast variation technique,suggesting a possibility of distinguishing thestatic disorder and dynamic ﬂuctuations (Fujiwara et al., in preparation).
To explore such a possibility of the contrast variation technique in neutron crystallography, we started a project of collecting
the neutron diﬀraction from crystals soakedin various fractions of D2 O. As a ﬁrst step, we
prepared a single crystal of proteins in H2 O,
原子炉：JRR-3

装置：BIX-4(1G-B)

and performed a trial measurement to see if
diﬀraction patterns could be collected.
A crystal of TAKA amylase was used in themeasurements. The crystal, grown in H2 O solution to the size of about 1 mm3 , belongs toorthorhombic P21 21 21 with cell dimensions of
a = 51 Å, b = 67 Å, and c = 133 Å. Diﬀraction images were collected at room temperature using monochromatic neutron beam (λ= 2.6 Å) and recorded on a neutron imaging
plate on a single-crystal diﬀractometer (BIX4) at JRR-3 in JAEA. We tried to record the
diﬀraction patterns under diﬀerent conditionsof exposure times and oscillation ranges. A
pattern collected by 8 hours exposure under
the no-oscillation condition showed diﬀraction
spots up to 9 Åresolution. This implies thatthe diﬀraction measurements are feasible on
single crystals in H2 O, but, for the measurements to be done within a reasonable machine
time, larger crystals with preferably smaller
cell dimensions will be required. Explorationof suitable crystals is underway.

Figure 1: Example of the diﬀraction patterns collected
at BIX-4.

References
1) P. A. Timmins and G. Zaccai: ”Eur. Biophys.
J.” 15, 257 (1988): P. A. Timmins: ”Neutron
Scattering in Biology” Springer, pp. 73-83 (2006).

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JAEA-Review 2011-050

1-6-10The State of Cryptobiosis of Larvae of Polypedilum Vandezplanki Studied by
Incoherent Inelastic Neutron Scattering
H. Nakagawa, T. Okuda1 and M. Kataoka
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki, 319-1195
Institute of Molecular and Cellular Biosciences, The University of Tokyo, Yayoi, Tokyo, 113-0032

Larvae of an African chironomid,
Polypedilum vanderplanki live in temporal rock pools and they can stand complete
desiccation in a cryptobiotic (ametabolic)state [1]. One of the most characteristic
phenomena is remarkable accumulation oftrehalose in the cryptobiotic larva. Slowlydehydrated larva (Slow sample) accumulated
suﬃcient trehalose successfully enters thestate of cryptobiosis, whereas quicklydehydrated one (Quick sample) with a small
amount of trehalose fails to do. It is suggested that the vitriﬁcation of the trehaloseis important for cryptobiosis. Generally the
glassy materials exhibits a glass transition.
This study aimed to examine the vitriﬁed
state in cryptobios in terms of glass transition
by incoherent inelastic neutron scattering
using slow and quick samples. The incoherent
neutron inelastic scattering experiments were
performed with the triple axis spectrometer,
TAS-2, in the JRR-3M reactor in Tokai.
The data were then collected at 100 and
280 K. Figure shows the inelastic neutron
scattering around the elastic peak of the slow
and quick samples of Larvae of Polypedilum
vandezplanki at 100 and 280 K. At 100
K signiﬁcant diﬀerence was not observed
between the slow and quick samples. At 280
K, the elastic intensity of the slow sample ishigher than that of the quick sample. Thissuggests that the relaxation process of theslow sample is inhibited and/or the timescalesof the process is slower than quick one. Thissuggests the appearance of a glass transition
with the quick sample, and the glassy statewith the slow one even in the physiologicaltemperature. These observations imply thatthe importance of the vitriﬁcation by thetrehalose for the cryptobiosis mechanism of
Larvae.
原子炉：JRR-3

装置：TAS-2(T2-4)

Figure 1: Inelastic neutron scattering around the elastic peak of the slow and quick samples of Larvae of
Polypedilum vandezplanki at 100 and 280 K.

References
1) T. Okuda et al. :“Proc.Arthropod.Embryol.Soc.Jpn”,39,1(2004).

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JAEA-Review 2011-050

1-6-11
Dynamical Transition of DNA Studied by Neutron Inelastic Scattering
H. Nakagawa, and H. Kono
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki, 319-1195

Protein recognize speciﬁc DNA sequences
not only through direct contact between
amino acids and bases, but also indirectlybased in the sequence-dependent conformation and deformability of the DNA [1]. Therefore, the relationship between DNA sequenceand its ﬂexibility should be known. MD simulation shows that DNA tetramer sequences
AATT and TTAA are conformationally morerigid and ﬂexible, respectively. This relationship should be conﬁrmed experimentally. In
this study, as a preliminary experiment, wemeasured the ﬂexibility of the hydrated DNA
with sequence of AATT (rigid sequence) by
incoherent neutron scattering. The neutron
scattering experiments were performed withthe triple axis spectrometer, LTAS, in the
JRR-3M reactor in Tokai with an energy resolution of 69 μ eV. The hydration level ofDNA sample is 0.49 g water/g DNA. Figure shows the temperature dependent atomic
mean-square displacement (MSD) of hydrated
DNA. As the temperature increase, the MSD
monotonously increases. At around 240 K,
DNA shows the sharp rise in the MSD. Thisis so called dynamical transition, which is generally observed with the hydrated biomacromolecules [2]. The slope of the regression lineof the temperature-dependent MSD gives theresilience of molecular structure as a force
constant [3]. Analytical equation is as below, k=0.00276/(d(MSD)/dT) [N/m]. Above
the transition temperature, the resilience ofDNA structure was estimated as 0.27 N/m.
This study demonstrated that neutron scattering experiment is applicable for estimating of DNA structural ﬂexibility. In the future, we will measure DNA with a sequenceof TTAA (ﬂexible sequence), and compare itwith AATT (rigid sequence).

Figure 1: The atomic mean-square displacement of thehydrated DNA with a sequence of AATT and the force
constant above the dynamical transition temperature
is 0.27 N/m.

2) W. Doster et al. :“Nature”,337, 754(1989).
3) G. Zaccai et al. :“Science”,288, 1605(2000).

References
1) S. Fujii et al. :“Nuc.Acid.Res”,35, 6063(2007).

原子炉：JRR-3

装置：LTAS(C2-1)

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JAEA-Review 2011-050

1-6-12
Glass Transition of Larvae of Polypedilum Vandezplanki Studied by Incoherent
Inelastic Neutron Scattering
H. Nakagawa, T. Okuda1 and M. Kataoka
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki, 319-1195
Institute of Molecular and Cellular Biosciences, The University of Tokyo, Yayoi, Tokyo, 113-0032

Larvae of an African chironomid,
Polypedilum vanderplanki live in temporal rock pools and they can stand complete
desiccation in a cryptobiotic (ametabolic)state [1]. One of the most characteristic
phenomena is remarkable accumulationof trehalose in the cryptobiotic larva.
Slowly-dehydrated larva (Slow sample) accumulated suﬃcient trehalose successfully
enters the state of cryptobiosis, whereas
quickly-dehydrated one (Quick sample)
with a small amount of trehalose fails to
do. It is suggested that the vitriﬁcation of
the trehalose is important for cryptobiosis.
Generally the glassy materials exhibit a glasstransition. This study aimed to examine
the vitriﬁed state in cryptobios in terms ofglass transition by incoherent elastic neutron
scattering using slow and quick samples. The
experiments were performed with the triple
axis spectrometer, LTAS, in the JRR-3M
reactor in Tokai with an energy resolutionof 61 μ eV. The data were then collected
at every 10 K between 100 and 290 K. The
q-dependence of the elastic intensity gives
the atomic mean-square displacement (MSD)
in the samples by Gaussian approximation
analysis. Figure shows the MSD of the slow
and quick samples of Larvae of Polypedilum
vandezplanki between 100 K and 300 K. As
the temperature increases, the MSDs of both
samples monotonously increase. At the lower
temperatures a signiﬁcant diﬀerence was notobserved between the slow and quick samples. The MSDs of the slow sample deviate
from that of the quick one above about 250
K, indicating the appearance of the glasstransition. This suggests that the relaxation
process of the slow sample is inhibited and/or
the timescales of the process is faster thanquick one. These observations imply that
原子炉：JRR-3

装置：LTAS(C2-1)

the importance of the vitriﬁcation by thetrehalose for the cryptobiosis mechanism of
Larvae.

Figure 1: Mean-square displacement of the slow andquick samples of Larvae of Polypedilum vandezplanki.

References
1) T. Okuda et al. :“Proc.Arthropod.Embryol.Soc.Jpn”,39,1(2004).

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JAEA-Review 2011-050

1-6-13Contrast Variation Measurements of Hen Egg White Lysozyme Amyloid Fibrils
S. Fujiwara, F. Matsumoto and H. Nakagawa
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Amyloid ﬁbrils, ﬁlamentous protein aggregates found in a wide variety of proteins, arethought to be related to pathogenesis of neurodegenerative diseases such as Altzheimer’s
disease and Parkinson’s disease. Understanding the mechanism of the amyloid ﬁbril formation is therefore important for the development of therapeutic strategies against theamyloid diseases. Moreover, since the amyloid ﬁbrils are found to be formed by proteins that have nothing to do with diseases, it
should be of considerable help to gain an insight into the generic properties of proteins related to the mechanisms of folding and stability. It was found that hen egg white lysozyme(HEWL) forms the amyloid ﬁbrils in highly
concentrated ethanol solution1) . The HEWLwater-ethanol system is suitable to study thegeneral mechanism of the amyloid ﬁbril formation. From small-angle X-ray and neutron
scattering (SAXS and SANS) measurements,
we showed that a pathway of the amyloid ﬁbril
formation of HEWL consists of three stages;
the formation of the dimers, the formation of
the protoﬁlaments, and the formation of theamyloid ﬁbrils via a lateral association of the
protoﬁlaments2)3) .
In order to understand the mechanism bywhich the amyloid ﬁbril formation occurs inmore detail, it is necessary to obtain detailed
structural information of each intermediate
structure. Here, we performed SANS experiments of HEWL solutions in 90% ethanol at
two HEWL concentrations, 2 mg/ml and 10
mg/ml, which correspond to the state where
protoﬁlaments are formed and the state where
the lateral association of the protoﬁlament
occurs, respectively. SANS curves of these
HEWL solutions, prepared in various fractions of deuterated solvents, were measured
with SANS-J at the guide hall of the reactor JRR-3M in JAEA, and cross-sectional
Guinier analysis was done to estimate the
原子炉：JRR-3

装置：SANS-J(C3-2)

cross-sectional radius of gyration at each contrast. Figure 1 shows the Stuhrmann plots4) ,the plots of square of the cross-sectional radius of gyration against a reciprocal of thecontrast, of these solutions. The data wereﬁt with a quadratic function of 1/(Δρ), suggesting that a center of the scattering density
shifts with contrasts. Detailed analysis withaid of model calculation is currently underway.

Figure 1: The Stuhrmann plots of the cross-section of
the amyloid protoﬁlament of HEWL. Filled and open
squares denote the data at 10 mg/ml and 2 mg/ml,
respectively.

References
1) S. Goda et al: ”Protein. Sci.” 9, 369 (2000).
2) Y. Yonezawa et al.: ”J. Mol. Biol.” 323, 237 (2002).
3) S. Fujiwara et al: ”J. Mol. Biol.” 331, 21 (2003).
4) H. B. Stuhrmann: ”J. Appl. Cryst.” 7, 173 (1974).

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JAEA-Review 2011-050

1-6-14
Small-Angle Neutron Scattering Measurements of Rhodanase-GroEL-GroES
ComplexK. Ichimura, Y. Matsuura1 , S. Fujiwara2 , Y. Kawata3 and H. Kihara1
Department of Biochemistry, Dokkyo University Medical Schoo, Mibu, Tochigi 321-0293
1
Department of Physics, Kansai Medical University, Hirakata 573-1136
2
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
3
Department of Biotechnology, Tottori University, Tottori 680-8552

When proteins are synthesized in vivo, they
are apt to fold with the aid of chaperon proteins. GroEL, a chaperon protein from E. coli,
forms hydrophobic bonds with the newly synthesized target protein, assisting the foldingof the target protein. In order to elucidate
the molecular mechanism of folding the target
protein with the aid of the chaperon protein,
it is important to elucidate various intermediate structures including the structure of thetarget protein when they are bound to chaperon protein, and the structure of GroEL in
the ternary complex formed with GroES. As
a ﬁrst step towards this purpose, we employedneutron scattering to investigate the structureof the target protein bound to GroEL.

wavelength of 6.5 Å(λ/Δλ=13.4%), and thesample-to-detector distance was 2.5 m. Temperature of the samples were kept at 15˚C during the measurements. Figure 1 shows the
SANS curve of d-rhodanase-GroEL-GroES,
that of h-rhodanase-GroEL-GroEs, and thediﬀerence curve between these two. Becauseof the unfortunate breakdown of the detector of SANS-J during our machine time, we
obtained only the curves with poor statistics. They, however, show that the reasonable diﬀerence curve were obtained, indicating that the SANS curve arising from rhodanase within the GroEL-GroES complex canbe extracted.

We used rhodanase as a target protein.
Rhodanase is a monomeric protein of themolecular weight of 33-kDa, and its folding
intermediate is known to bind to GroEL. Employing the mutated GroEL1) , which forms
stable complex with the target proteins andbinds GroES at its complex with the target
protein, made it possible to measure smallangle neutron scattering (SANS) curves of
the rhodanase-GroEL complex. We prepared
deuterated (d-) and undeuterated (h-) rhodanase, and mixed with GroEL and GroES
at 1:1:1 stoichiometry in solvent containing
42% D2 O, at which the scattering length density of the solvent was matched to that of the
undeuterated proteins.
We measured SANS curves of d-rhodanaseGroEL-GroES complex and h-rhodanaseGroEL-GroES complex with the Small-Angle
Neutron Scattering Instrument (SANS-J) at
the guide hall of the reactor JRR-3M in Japan
Atomic Energy Agency. The measurements
were done with the incident neutrons of the
原子炉：JRR-3

装置：SANS-J(C3-2)

Figure 1: SANS curves of d-rhodanase-GroEL-GroES,
h-rhodanase-GroEL-GroES, and the diﬀerence curves.

References
1) Y. Kawata et al: ”Biochemistry” 38, 15731 (1999).

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JAEA-Review 2011-050

1-6-15
Small-Angle Neutron Scattering Measurements of α-Synuclein and its
Disease-Related Mutants
1,2,, H.
H. Mochizuki
Mochizuki11,, T.
T. Yasuda
Yasuda11,, J.
J. Yamagucghi
Yamaguchi11,, Y.
Y. Mizuno
Mizuno11,,S.
S. Naito
Naito1,2
3
2
2
M. Furusaka , S. Ikeda , M. H. Shimizu and S. Fujiwara4
1

Dept. of Neurol., Juntendo Univ. Sch. of Med.,Tokyo 113-8421
2
KEK, Tsukuba, Ibaraki 305-0801
3
Dept. of Mech. Intell. Eng., Grad. School of Eng., Hokkaido Univ., Sapporo 060-8628
4
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Parkinson’s disease (PD) is a neurodegerative disorder that is characterized by the lossof dopaminergic neurons from the substantia
nigra, and the formation of ﬁbrillar intraneuronal inclusions called Lewy bodies, the major
component of which are ﬁlaments consistingof α-synuclein. It has been postulated thatthe ﬁbril formation by α-synuclein is closely
associated with pathogenesis of PD. In particular, the facts that α-synuclein found in
the ﬁbrils in Lewy bodies is phosphorylated
at the residue Ser129 and that missense mutants of α-synuclein (A30P and A53T), foundin the patients of rare, autosomal dominant
early-onset PD, form ﬁbrils imply that ﬁbril formation induced by abnormal state of
α-synuclein is associated with PD. It is thus
important to investigate relationship between
the structural states of α-synuclein and ﬁbril
formation.
As a ﬁrst step towards this purpose, we prepared three kinds of samples; the wild-type αsynuclein, the mutant A53T, and the mutant
S129D, which mimics the phosphorylation at
this residue, and investigate the structuresof these proteins in solution. We employedsmall-angle neutron scattering (SANS). We
prepared the solutions containing these proteins under the condition where the ﬁbril formation does not occur, and SANS curves ofthese solutions were measured with the SmallAngle Neutron Scattering Instrument (SANSJ) at the guide hall of the reactor JRR-3M inJapan Atomic Energy Agency. The measurements were done with the incident neutronsof the wavelength of 6.5 Å(λ/Δλ= 12.9%),and the sample-to-detector distance was 6 m.
Temperature of the samples were kept at 20˚C
原子炉：JRR-3

装置：SANS-J(C3-2)

during the measurements.
Figure 1(a) shows the SANS curves of thewild type α-synuclein, the mutant A53T, andthe mutant S129D. Diﬀerences in the SANS
curves are clearly observed between the wild
type, A53T, and S129D, indicating the structural diﬀerences in these proteins. Figure 1(b)shows the Kratky plots of these SANS curves.
Linear increases with increasing Q imply thatthese proteins have a random-coil like conformation rather than a globular structure. The
diﬀerences in the plots appear to be consistent
with the development of the beginnings of atightly packed core in the mutants. Detailed
analysis is currently underway.

Figure 1: (a) SANS curves and (b) Kratky plots of
the wild type α-synuclein, the mutant (A53T), andthe mutant (S129D).

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JAEA-Review 2011-050
















1.  ਛᕈሶᢔੂ 7 ၮ␆‛ℂቇ㨯ਛᕈሶశቇ


1. Neutron Scattering

7 Fundamental Physics㨯Neutron
Optics㪄㩷 㪉㪎㪐㩷㪄This is a blank page.

JAEA-Review 2011-050

1-7-1

Development of phase correction devices for high resolution NRSE spectrometer
Kitaguchi M.(A), Hino M.(A), Kawabata Y.(A), Hayashida H.(B), Tasaki S.(B),Maruyama R.(C), Ebisawa T.(C)KURRI(A), Kyoto Univ.(B), JAEA(C)Neutron spin echo (NSE) spectrometer is
one of the techniques with the highest
energy resolution for quasi-elastic scattering[1]. In the case of spin echo the beam
divergence makes the deviation of the relative phase between up- and down-spincomponents, which is equivalent to spin
precession, because the relative phase is
proportional to the neutron ﬂight length.
The deviation of the phase can be corrected by using three magnetic ﬁelds withthe strength which is proportional to thesquare of the radius. In the conventional
NSE with the spin quantization axis along
to the beam direction, such magnetic ﬁelds
are made with Fresnel coils [2]. In neutron
resonance spin echo (NRSE) spectrometer[3], however, the spin quantization axis is
generally transverse to the beam. Magnetic
ﬁelds for adiabatic transition of the quantization axis for the correction with Fresnel
coils make the vertical asymmetric distribution of the ﬁeld integral. That makes thecontrast of spin echo signal disappear.
We consider the devices which make thetransition of spin quantization axis onlyat the resonance spin ﬂippers (RSFs). The
quantization axis of the incident neutronschanges from longitudinal direction into
vertical direction just before a RSF. Afterthe ﬂip of the spin, the quantization axischanges to longitudinal direction. We callthe devices which provides the transition
ﬁeld as ”coupling coils”. By using a set of
coupling coils provides parabola distribution of ﬁeld integral, which is the same representation as the correction ﬁeld only forthe vertical divergence. Numerical simulation of the phase distribution for the beam
divergence was performed for the system
including coupling coils. We demonstrated
that the phase through the system can be
uniform for the wide beam divergence. Test

experiments are in progress at cold neutron
beam line MINE1 and MINE2.
References[1] F. Mezei: Z. Phys. 255 (1972) 146.
[2] F. Mezei: The Principles of Neutron spin
echo, proceedings of the ILL Workshop,
Grenoble 1979, Lecture Notes in Physics,
vol. 128, Springer, Heidelberg, 1979, pp. 326.
[3] R. Gaehler, R. Golub: Z. Phys. B65 (1987)
43.
[4] M. Kitaguchi, et. al., Meas. Sci. Techno.,
to be published in 2008.

Fig. 1. Top: Concept of coupling coils. Bottom: Simulation of the phase distribution for beam divergence. The phase is uniform for wide beam divergence at a proper set of current for the coupling
coils.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 425

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Development of Jamin Type Cold Neutron Interferometerwith Completely Separated Two Paths
1,4 Y. Seki, 1 K. Taketani, 2 H. Funahashi,

3 M. Kitaguchi, 3 M. Hino, 4 Y. Otake, 5 H.M. Shimizu

Department of Physics, Kyoto University, Kyoto 606-8502, Japan
Osaka Electro-Communication University, 18-8 Hatsucho, Neyagawa, Osaka 572-8530, Japan
Research Reactor Institute, Kyoto University, Kumatori, Sennan, Osaka 590-0490, JapanRIKEN, 2-1 Hirosawa, Wako, Saitama 351- 0198, Japan
KEK, 1-1 Oho, Tsukuba, Ibaraki 305-0801, JapanWe are developing large-dimensional
cold-neutron interferometers with multilayer mirrors in order to investigate smallinteractions.
The success of Jamin-type interferometer made up of two ’beam splitting etalons(BSEs)’ [Fig. 1] with a 10 μm gap have conﬁrmed the accuracy of manufacturing of
etalons. However, even if the beam width
was collimated to 100 μm, the two beams
were almost overlapped. When we enlarge the gap of the BSE up to 200 μm, we
can separate the beam spatially and realize
various experimental conﬁguration, for example, inserting the some devices between
paths of the interferometer.
One of our experimental targets isthe precision measurement of AharonovCasher effect. The AC effect is a dualof the Aharonov-Bohm effect. When aneutral particle with a magnetic moment
goes around change density the topological phase shift is induced. The AC phaseshift was detected for the ﬁrst time by using the Si crystal neutron interferometer,
however, the observed value was inconsistent with the expected value. Our largedimensional cold-neutron interferometerwith separated long paths can measure
the topological AC phase shift precisely
enough.
The development is performed at coldneutron beam line MINE2 at JRR-3M reactor in JAEA. The beam has a wave lengthof 0.88nm and a bandwidth of 2.4% in
FWHM. The typical longitudinal, verticaland horizontal coherence lengths in our
setup are about 17 nm, 50 nm and 2 μm,

respectively. Therefore the tolerances foralignment of two BSEs are
α < 40μrad,

β < 130

μrad,

(1)

where α and β are the relative angle between two BSEs in the horizontal and vertical planes, respectively.
In order to arrange BSEs meeting thiscoherence condition, we have developed
a new jig employing a precise planar
substrate (SIGMA KOKI OFPXP-150S20-4).
The 150-cm-square substrate is made of
PYREX with ﬂatness of λ He− Ne /4. Each
BSEs was ﬁxed closely to the substrate at
three points with screws. We have obtained reasonable signals of the interference fringe, and are trying to ﬁnd a way tostabilize and improve its contrast.
In addition, we studied the thermal,
magnetic and vibration stability in the experimental environment. It was understood that phase drifts of neutron spin interferometry (∼ 34 mrad) were almost followed by the magnetic ﬂuctuations (∼ 16
mG).
References[1] M. Kitaguchi et al.: Phys. Rev. A 67
(2003) 033609.

Fig. 1. Jamin-type interferometer with two BSEs

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 456

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1-7-3

Development of beam splitting etalons for pulsed neutrons II
Kitaguchi M.(A), Seki Y.(B), Taketani K.(B), Funahashi H.(C), Hino M.(A), and Shimizu
H. M.(D)(A)KURRI, (B)Kyoto Univ., (C)Osaka Electro-Comunication Univ., (D)KEK
A large dimensional interferometer forlong wavelength neutrons has the advantage to increase the sensitivity to smallinteractions. Multilayer mirror is suitable for Bragg reﬂection of cold neutrons. We demonstrated Jamin-type interferometer for cold neutrons using beam
splitting etalons (BSEs), which enables
us to align the four independent multilayer mirrors in the interferometer withinrequired precision [1]. We are preparing for high-resolution measurement of
Aharonov-Casher effect [2,3] by using thistype of interferometer.
The interferometer for pulsed neutrons
can increases neutron counts available forAC measurement because the phase shift
is independent from the velocity of incident neutrons. Neutron interferometerwith multilayer mirrors can be applied
to pulsed neutrons by replacing the mirrors with supermirrors. The supermirrors
can reﬂect neutrons with wide range of
wavelength at a proper incident angle. In
the case of neutron spin interferometer of
Jamin type, a magnetic supermirror on the
one plane of the BSE reﬂects only up-spincomponent of the neutrons and a nonmagnetic supermirror on the other planereﬂects transmitted down-spin component.
The second BSE with supermirrors recombines the two components. High polarization of both of reﬂected and transmitted
beam for magnetic mirror is required in order to split the beam into two paths according to the spin states.
We deposited magnetic supermirrors on
silicon wafers by using both of ion beam
sputtering instrument and vacuum evaporation instrument at KURRI for test of BSE.
The reﬂectivity of the magnetic supermirrors were measured by scanning of incident angle instead of neutron wavelength.

Test experiments were performed using thecold neutron beam line MINE2 at the JRR3M reactor in JAEA. The beam had a wavelength of 0.88 nm and a bandwidth of 2.7%
in FWHM. The magnetic mirrors required
external magnetic ﬁeld for magnetic saturation of the mirror. Strong magnetic ﬁeld
in local area in neutron spin interferometer would decrease the visibility of interferogram due to depolarization or deviationof the relative phase between the two spinstates. We are continuing the developmentof the magnetic supermirror for lower external ﬁeld. The interferometer for the ACmeasurements must have perfectly separated two paths enclosing an electrode. We
are also continuing on the constructing ofinterferometer using BSEs with large gaps.
References[1] M. Kitaguchi et al.: Phys. Rev. A 67
(2003) 033609.
[2] Y. Aharonov and A. Casher: Phys. Rev.
Lett. 53 (1984) 319.
[3] A. Cimmino et al.: Phys. Rev. Lett. 63(1989) 380.

Fig. 1. Reﬂectivity of multilayer spin splitter withthe magnetic supermirror. Because the mirror was
not saturated, the reﬂectivity for up-spin was nothigh for BSEs.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 565

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1-7-4

Possible improvement of thin magnetic ﬁlm using Pd
Seiji Tasaki, Satoshi Kuramoto, Yutaka Abe, Masahiro Hino
Department of Nuclear Engineering Kyoto University
Multilayers consisting of alternative stack ofa magnetic material and a non-magnetic material is widely used as neutron spin polarizers.
Such multilayers are also a key element for consisting multilayer spin splitter, consisting of polarizing mirror, gap layer and reﬂection mirror,
which can be used to measure precise quantityof absorbed material by the gap layer material.
One way to the improvement of polarizing
efﬁciency of the multilayer polarizer is to makethe saturated magnetic ﬁeld higher. Higher
ﬁeld strength allows us higher potential contrast between neutron eigenstates, and higher
reﬂectivity for neutron with ﬁeld-parallel spin.
Recently, Noma et al. [1] reported that saturated magnetic ﬁeld of FeCo was increased
by being sandwiched by Pd thin ﬁlms. In thepresent study, we studied the effect of Pd thinlayer over Fe ﬁlms in polarizing multilayers.
The samples are fabricated with vacuum
evaporation. Firstly combination of thicknessof Pd and Fe layers is investigated. Multilayers with various combination of Pd and Fe suchas (1nm, 4nm), (1nm, 5nm), (1nm, 6nm), (2nm,6nm), (3nm, 6nm) where total Fe thickness isequal to 60nm were fabricated and their magnetization is measured with vibrating magnetometer. The thickness of the ﬁlms are measured with X-ray reﬂectometer. Combinationof 3nm-Pd and 6nm-Fe gave highest magnetization. Measured magnetic ﬁeld is 1.51 T whichis reasonable value comparing with bulk magnetization of 2.1 T for density reduction of 75%
given by X-ray reﬂectivity.
Secondly, for comparison, various combination of Fe and other material was tested. HereGe, Ti, Si were adopted other than Pd. The
thickness of all non magnetic material is 2nm,
and that of Fe is 6nm. The calibrated hysteresis
curves are shown in the upper ﬁgure in Fig.1.
Here Ge gives similar result as Pd. However,Pd gives a little higher ﬁeld and smaller coercive force. These saturated magnetization was
also conﬁrmed with polarized neutron reﬂectivity.

The lower ﬁgure in Fig.1 shows polarized
neutron reﬂectivity of Fe6nm-Pd2nm-Ge2nmPd2nm multilayer with 15 period. The rise of
reﬂectivity in the region Qz > 0.06 is due to theposition dependent back ground. Other than
this region, the reﬂectivity is well reproducedby the calculation in which saturated magnetic
ﬁeld is assumed as 1.51T.

Fig. 1. The caribrated hysteresis curves of multilayers of Fe and various material (upper), and polarized neutron reﬂectivity of Fe6nm-Pd2nm-Ge2nmPd2nm multilayer with 15 period (lower).

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 599

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1-7-5

Development of neutron optics with a curved supermirror
Ikeda K., Sato H., Hirota K., Mishima K.
Radiation Laboratory, RIKEN, 2-1 Hirosawa, Wako, 351-0198
We are developing real curved supermirror, which is deposited neutron supermirror on the substrate with a curved surface.
First in our sputtering machine, we manage to keep the uniformity of layer thickness over the large area of tens to a hundred centimeter for large substrates withﬂat surface. But, when the curvature of surface is large and the surface is not considered to be ﬂat, it’s not easy to deposit supermirror uniformly on the curved surface as
we can do on ﬂat substrate. We then haveto make the layer-thickness distribution tohave conformity to curved surface, or ﬁnd
the way to compensate for the distribution.
We, at ﬁrst, made the mask which is themeshes with stainless wires of 0.3mm in diameter in order to keep the uniformity oflayer thickness over 300mm long area. Twokinds of meshed patterns and blank area
were used for 300mm long substrate. Fig.
1 shows the sputtering rate in the case ofwith the mask and without the mask versus the position on the sample stage of our
sputtering machine. The position x=0 is
the center of the stage. We succeeded todecrease the differences of layer thickness
from 28% to 4% between the center and theedge on the sample stage.
Second, we deposited 2.5Qc supermirror
on the substrate with an ellipsoidal surface
on which substrate 2.0Qc supermirror was
requested. The performance of 2.5Qc to
2.0Qc supermirror was kept at the thinnest
area to the thickest area, since the maximun reduction of the layer thickness wasestimated to be 27% in the ellipsoidal surface. Fig. 2 shows the neutron reﬂectivity of 2.5Qc supermirror fabricated with themask. The mirror has the performance of
2.1Qc supermirror and the neutron reﬂectivity at 2.0Qc was 95%. The supermirror
is deposited on a ﬂut substrate of Si at thecenter of the sample stage.

Next, we have to ﬁnd the way to keep
uniformity of layer thickness on the surface with large curvature. The larger distribution of layer thickness yields stronger
stress in the layers. It thus results in the
peeling layers off the substrate and prevents from developing higher-Qc supermirror with curved surface.

Fig. 1. Sputtering rate in the case of with the mask
(circles) and without the mask (squares) versus the
position on the sample stage of our sputtering machine. Fig. 2. Neutron reﬂectivity of 2.5Qc supermirror fabricated with the mask.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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Thermal diﬀuse scattering eﬀect on neutron holography
K. Hayashi, K. Ohyama, S. Orimo, Y. Nakamori, H. Takahashi 1 and K. Shibata 2
1 IMR, Tohoku Univ., 2 Graduate School for Environmental Science, Tohoku Univ., 3 JAEA
In the previous experiment, we measured
efﬁciently the neutron hologram of a palladium hydride single crystal using thepowder diffrcatometer of HERMES in JRR3M reactor, and found the thermal diffuse scattering effect in the measured hologram.1) In this study, we used again a palladium hydride single crystal as the measured sample and evaluated the temperature dependence of the sample on the thermal diffuse scattering in the hologram. The
sample dimension was 10 mm in a diameter and 5 mm in a thickness, and it wascoated by Cu not to desorb the hydrogengas. Wavelength of the neutron was 0.182
nm. Sample was rotated in the range of
0 - 359 deg with the step of 1 deg, whererotation axis was parallel to the incoming beam direction. Neutrons incoherently
scattered by hydrogen nuclei in the sample were detected by HERMES 150 He3
counters at each sample rotation angle. Polar angle of the measured hologram deﬁned by the counter ranged from 7 deg to
157 deg. Dwelling time at each angle was
480 sec. The average neutron intensity ateach pixel was about 500 counts. To reduce the effect of thermal diffuse scattering
the cryostream cooler (Oxford: cryostream
70 series) was used for keeping the sample temperature at 100 K. Figures 1 (a)and (b) show the 2D angular distributionsof the neutron intensities around the sample at room temperature and 100 K, respectively. The observed data were four-foldsymmetrized using sample crystal symmetry in order to suppress statistical error, andthen they were low-pass ﬁltered. The displayed patterns exhibit strong spots reﬂecting the sample crystal symmetry, due tothermal diffuse scattering. However, thecontrast of the pattern in Fig.1 (b) is weaker
than that in Fig. 1 (a). Figure 1 (c) shows
the intensities changes as a function of az-

imuthal angle at polar angle of 80 deg. The
amplitude of the intensity change at room
temperature was twice as much as that at
100 K. These results revealed that the effect of the thermal diffuse scattering effect
was reduced by the sample cooling.
1) K. Hayashi, K. Ohoyama, S. Orimo, Y.
Nakamori, H. Takahashi and K. Shibata,Jpn. J. Appl. Phys. in press.

Fig. 1. Fig.1 2D angular distributions of the neutron
intensities around the sample. (a) room temerature.
(b) 100 K. (c) Intensities change at polar angle of 80
deg.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 427

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1-8-2

Development of A New Spin-Phase Contrast Imaging of Neutron
Seiji Tasaki, Masashi Kageyama, Masahiro Hino, Yuji Kawabata
Department of Nuclear Engineering Kyoto University
Spin-phase contrast imaging is a methodof taking 2D image of the phase difference between spin-eigenfunctions of neutron. Since the phase difference is proportional to the magnetic integral along
the neutron trajectory, the image shows themagnetic ﬁeld distribution over the beamcross section.
The phase difference between the spineigenfunctions is measured using neutron
spin interferometer (NSI), installed at C31-2-2 port of JRR-3M reactor in JAEA.
In NSI, neutrons monochromated with
8.8Å(Δλ/λ = 2.7%) is polarized and ischanged into superposition state of spinparallel and antiparallel eigenstate to theguide magnetic ﬁeld by π/2-ﬂipper. In
the middle of the set-up, the spin stateof neutron is reversed by π-ﬂipper, in order to realize spin echo of neutron, withwhich additional phase difference caused
by outer magnetic ﬁeld can be canceled.
Then after going through the sample, neutron comes to the second π/2-ﬂipper andspin-analyzer, where the measured neutron counts are proportional to the cosineof phase difference. Available beam area is
2mm(w)×20mm(h).
In the experiments, neutron counts aremeasured via additional phase φ, thecounts are ﬁtted to A(1 + cos(φ0 + φ)) and
φ0 is the desired phase difference. In thepresent study, the additional phase is introduced as phase difference of rf-current to
π/2 and π-ﬂipper.
As neutron detector, we adopt 2D Photo
Multiplier with Li-glass scintillator andneutron imaging plate (IP). The former has
real-time read out system but low spatial
resolution, where the latter has very highresolution but requires off-line read out.
With the former detector, we made preliminary experiments and conﬁrmed therelation between magnetic ﬁeld and phasedifference in the case of magnetic coils (viaelectric current) and magnetic thin layer(via incident glancing angle).
With the IP, neutron imagines for different additional phase is recorded in a single
IP. An example is shown in Fig. 1. The
left picture is the sample, which is a 6Q polarizing supermirror with total thickness ofmagnetic layers is about 6μm. The sample
was kept in non magnetic atmosphere formonths. Hence the sample was demagnetized gradually. Left picture in Fig.1 is aphotograph of the sample. Middle picture
is normal transmission image, where noclear image is shown since almost all neutrons are transmitted. Right picture is thephase image, where inhomogeneous distribution of magnetic ﬁeld is shown.

Fig. 1. The results of the spin-phase contrast imaging of neutron using imaging plate.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 575

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1-8-3

Development of transmittion geometry supermirror polarizer
M.Hino, M.Kitaguchi, H.Hayashida1 , Y.Kawabata, S. Tasaki1
KURRI, 1 Depart. Nucl. Eng., Kyoto Univ.

Magnetic multilayer mirror consisting of
ferromagnetic layers and nonmagnetic layers is useful to polarize neutron beam. Polarizing supermirror is a stack of magnetic
multilayer with gradually increasing valueof the d-spacing. Polarizing supermirror isstable and it is easy to handle as neutron
polarizer. Recently performance of He-3
spin ﬁlter is improved and it is better thansupermirror when we need analyzer covering wide scattering angle for thermal neutron. When we use cold neutron and polarizer covering narrow beam cross section,
polarizing supermirror is more useful than
He-3 spin ﬁlter since transmission probability of supermirror is better than that ofspin ﬁlter.
Recently we succeeded in fabricating
m=4.9 Fe/Ge polarizing supermirror byusing ion beam sputter (IBS) machine at
KURRI[1]. The magnetic property of supermirror is better than Fe/Ge and Fe/Si
ones by inserting thin Si layer in which
thickness 0.5 nm between Fe and Ge layer.
The measurement was carried out at C3-12-3 port (MINE2) at JRR-3M at JAEA. The
average wavelength of incident neutron is
0.88 nm and the resolution is 2.7 % in full
width half maximum. The divergent angleof neutron beam was smaller than 1 mrad.
The strength of external magnetic ﬁeld is 45
mT. The reﬂectivity and polarization efﬁciency of reﬂected neutron is estimated to
be above 0.7 and 0.94, respectively. The
reﬂectivity is very high, however, the polarization efﬁciency of transmitted neutronis 0.5. Because polarization efﬁciency oftransmitted neutron Pt is related reﬂectivity R and it is given by the following equation Pt  Pr R/(2 − R), where Pr is the polarization efﬁciency of reﬂected neutron.
The transmission geometry supermirror
polarizer does not change neutron beamline and it is more useful and it is importantfor development of transmission geometry
supermirror polarizer (analyzer) to enlarge
utility of polarized neutron beam. Thus westarted to develop transmission geometry
supermirror polarizer.
The supermirrors were deposited on silicon wafer (150x60x0.6mm3 ) using IBS at
KURRI. The measurement was carried out
at C3-1-2-2 port (MINE1) at JRR-3M at
JAEA. The average wavelength of incident
neutron is 0.81 nm and the resolution is 17.4
% in full width half maximum. The divergent angle of neutron beam was 1.9 mrad.
The strength of external magnetic ﬁeld is
60 mT. As shown in Fig.1, we succeededin fabricating m=4 transmission geometry
polarizing supermirror. The ﬂipping ratio
is higher than 20 at 2lemle4.1 and it is especially higher than 70 at 1.4lemle2.6. As anext step, we will improve the ﬂipping ratio at mge2.6.
[1] M.Hino, et al., ISSP Activity Report, Vol. 13 ,ibid, Physica B (2006) 385386(2006)1187.

Fig. 1. Fig.1 Measured transmittion probabilities of up (blue) and down(red) spin neutron for
m=4 Fe/SiGe3 (Si:0.5nm) magnetic supermirror. The
green line indicates ﬂipping ratio that transmittion
probability of down spin neutron devided by that ofup spin one.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 627

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1-8-4

Observation of superparamagnetic ﬂuctuations in magnetic ferroﬂuid using MIEZE
spectroscopy
M.Hino, H.Hayashida1 , M.Kitaguchi, N.Achiwa2 and Y. Kawabata
KURRI, 1 Depart. Nucl. Eng., Kyoto Univ.,2 Grad. Sch. Sci., Osaka Univ.
We have developed a MIEZE(Modulated
IntEnsity by Zero Effort) spectrometer at
C3-1-2-2(MINE1) port JRR-3M in order toinstall it to the high ﬂux pulsed neutron
source at J-PARC in the near future. In the
MIEZE spectrometer the sample is placed
after the analyzer and there are no opticalcomponents between sample and detector.
When we measure NSE and NRSE signals
on paramagnetic and ferromagnetic samples the maximum contrast is reduced to
0.5 or less. On the other hand the contrast
of a MIEZE signal can be observed withalmost 100 % contrast(1) even in magnetic
scattering because the sample is placed after the analyzer. MIEZE signal is sensitive for dispersion of neutron trajectories
from sample to detector. In other words
MIEZE signal is reduced due to the dispersion alone even without in- and quasielastic scattering. We studied the correlation between experimental conﬁgurationand its resolution function using Monte
Carlo simulation. We prepared a magnetite
ferroﬂuid sample and examined the simulation model by experiments. The experimental results were reproduced withthe simulation [1]. We studied dynamical structure-changes of the magnetite ferroﬂuid by using the MIEZE spectrometer.
The ferroﬂuid consists of magnetite particles and solvent (heavy water). The magnetite particles with a diameter in the orderof 10 nm are coated by oleic acid. There are
two kind of dynamic modes in ferroﬂuid.
One is diffusion of magnetite particles andthe other is superparamagnetic ﬂuctuation.
When we observe the superparamagnetic
ﬂuctuation, we have to measure spin-ﬂip
scattering from magnetite particle. The
intensity of magnetic scattering is muchsmaller than nuclear scattering and separate spin-ﬂip and non-spin-ﬂip scattering.

Thus we placed second analyzer after sample in order to observe spin-ﬂip scattering only. The second analyzer is transmission geometry magnetic supermirror tokeep trajectories of scattering neutron. Figure 1 shows typical MIEZE signals with
nuclear and spin ﬂip(magnetic) scattering
at Q=0.68 nm−1 at room temperature. As
shown in Fig.1, the contrast of MIEZE signal with magnetic scattering reduced andwe succeeded in observing superparamagnetic ﬂuctuation.
[1] H.Hayashida, et al., Measurement Science and Technology (2008), in press.

Fig. 1. Fig.1 Measured MIEZE signal(Q=0.68nm−1 )with (a) nuclear and (b) magnetic scattering in magnetic ferroﬂuid. (c) Measured MIEZE signal withoutsample.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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1-8-5
Installation of a prototype of focusing-type small-angle neutron scattering
instrument with an ellipsoidal supermirror
M. Furusaka(A), T. Satoh(B), Y. Sasaki(A), Y. Kawamura(C), T. Asami(C), Y. Otake(D),K. Ikeda(D), P. Mikula(E), Y. Kiyanagi(A), S. Naito(F), H. Yoshizawa(C)(A)Grad. Sch. Eng., Hokkaido Univ. , (B)KUR, Kyoto Univ., (C)ISSP Univ. Tokyo, (D)RIKEN,(E)NPI, Czech Republic, (F)KENS, KEK
SANS is a very powerful and popular technique to study nano-scale structure in matters. Every neutron facilities all over theworld have at least one or two such instruments, but very often, they are oversubscribed and not so easy to obtained machine time on these machines. We, therefore, decided to develop a prototype sansinstrument, that is compact and low cost,hence can be easily installed at any neutron
beam line.
Using a compact ellipsoidal mirror asa focusing device and high positionalresolution detectors, which have beendeveloped in the last decade, we can
now construct very compact and versatile focusing-type SANS instruments. We
are now developing such instruments, andnamed it ”Mini-focusing small-angle neutron scattering instrument (mfSANS)”.
At ﬁrst, we have conducted mock-up
test experiments of a time-of-ﬂight typemfSANS at a small pulsed cold-neutron
source facility at Hokkaido University. The
results looked very promising: from thepreliminary results showed that we could
measure minimum momentum transfer Q
of the order of 2 × 10-2 nm-1 if the sample
is a strong scatterer.

tector, is only about 2.8 m. It is installed not
horizontally, but installed above the beamline at the angle of 135 ° (45 °) from thehorizontal line. Aperture size of 1 to 10 mm
can be selected remotely. A focusing mirror of 900 mm in length was used, thathas a curved surface of a part of an ellipsoid of 2.5 m major and 20 mm minor axes,
coated with 2.5 Qc supermirror. It is divided into three parts, each with 300 mm inlength. Sample position is just after the mirror. A detector of 5 inch effective diameterthat consists of a resistive-wire type photomultiplier with a ZnS scintillation plate isused. The position resolution of it is lessthan 1 mm.
Several very preliminary data were obtained with the instrument. Unfortunately,slight miss-alignments in the focusing mirrors were found. Even though, the missalignments were not so large, the direct
beam focusing position was displaced byabout 300 mm and it was blurred by almost a factor of 2. Even with such a geometry, we could measure fairly good smallangle scattering patterns and minimum Q
of about 0.05 nm-1 using 2 mm aperture.
Because of the long shutdown of the JRR3 reactor, we will resume commissioning
from July, 2008.

We have just ﬁnished a ﬁrst phase construction of another prototype mfSANS instrument at the JRR-3 reactor at C1-3 position in October as shown in the ﬁgure. We
put a new monochromator at just downstream of the ULS (ultra low-angle scattering) instrument in the same monochromator shielding. The total length of the instrument, from the monochromator to the deActivity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
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JAEA-Review 2011-050

Fig. 1. Mini-focusing small-angle neutron scattering
instrument (mfSANS) just installed above the ULS
monochromator shielding.

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1-8-6

Development of 10 GPa class cubic anvil type high pressure apparatus for neutron
scattering experiments
Tetsuya Fujiwaraa , Kazuyuki Matsubayashib , Yoshiya Uwatokob , Naofumi Asob ,Masakazu Nishib , Hideki Yoshizawaba Yamaguchi Univ., b ISSP, Univ. of Tokyo
Over the past few decades, a considerable number of studies have been devoted
the physical properties of Ce-, Yb- and Ubased intermetallics, the so-called strongly
correlated electron systems. In these systems, an external pressure is often a key tobring about a new type of ground state accompanied with exotic physical phenomena, such as a heavy fermion superconductivity or valence transition and so on.
Accordingly, nowadays the concern with
an application of high pressure generation
techniques to various sorts of experimental measurements has been growing remarkably. In this work, we have developed a cubic anvil type high pressure cell(CAC). CAC can generate superior hydrostatic pressure to other high pressure apparatuses. In CAC, however, sample spaceis surrounded and enclosed by thick sliding anvil blocks made of tungsten carbide(WC) whose neutron transmittance is remarkably poor. So, to optimize CAC forneutron scattering experiments, We conducted a review of apparatus volume anda material of anvil block. Consequently,
we succeeded in reducing the diameter ofcell from 180 mmφ to 80 mmφ and the massof apparatus from 26.8 kg to 1.4 kg. Fig.
1 is photograph of downsized CAC. Furthermore, anvil block made of ZrO2 withsuperior neutron transmittance to WC was
prepared. Pressurization examination was
performed at room temperature. Daphne
7373 and a single crystal of NaCl wereused as a pressure transmitting medium
and a manometer, respectively. Transmittance of apparatus keeps up above ∼ 30 %.
At present, applying external load, pressure distribution brings about materially,so that an intensity of NaCl (200) Bragg

reﬂection remarkably decreases. There isroom for improvement in homogenizationof generated pressure.

Fig. 1. Downsized Cubic anvil type high pressure
cell optimized for neutron scattering experiments

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 658

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JAEA-Review 2011-050

1-8-7

Development of Large 2D-PSD under collaboration with HANARO
Y. Noda, M. Watanabe, H. Kimura, Y. Dohi, Y. Ishikawa, T. Yamazaki, M. Moon(A) andChang-Hee Lee(A)IMRAM, Tohoku University, Katahira Sendai 980-8577, (A)HANARO, KOREA ATOMICENERGY RESEARCH INSTITUTE ,Taejon, 305-600, Korea
We have developed a large-scale two dimensional position sensitive detector (2DPSD) under the collaboration with HANARO of KAERI. First, we have tested asmall and ﬂat 2D-PSD to evaluate the capability of the counter. The size of thisplot-type detector is about 20cm x 20cm.
Then, we have developed more realistic
size detector to evaluate the capability, especially to apply structure analysis of relatively complicated system. The detector isbend one and size of this prototype detector is 63cm x 44cm. The upper panel of Fig.
1 shows the settlement of the 2D-PSD at T22 beam port.
First, we settled a Laser beam to adjust
to the neutron beam path of FONDER.
Then, goniometer with 4K-cryostat is puton the beam. This Laser beam evaluatessample position. The simple example
to test oscillation photograph is that ofNaCl, and shown in the lower panel ofFig.1. Condition of measurement is thefollowing: omega speed is 0.2 degree/min.
Each 0.4 degree, data is transferred to computer. All of parameters of 2D-PSD were
determined by using the standard NaCl
crystal. As shown in Fig.1, we can see thelayer structure of NaCl from L=-1 to L=+2.
We have developed new program to ﬁndpeak position and intensity automatically.
Peak position gives reasonable good lattice
parameters. Then, we tried measurementsof various crystals. Still we are developing
new programs to do precise structure analysis. It seems to get good data from very
efﬁcient experiment. The lattice parameterof NaCl obtained by 2D-PSD is ; a=5.644(6)b=5.638(8) c=5.644(22)[A] alpha=89.8(2)beta=90.2(2) gamma= 90.2(2)[deg] vol.=179.6(8) [Aˆ3] These numbers can be compared with those taken by using FONDER: a=5.6569(11) b=5.6566(7) c=5.6542(45)[A]alpha=89.99(3) beta=89.92(3) gamma=
89.99(1)[deg] vol.=180.93(15) [Aˆ3]. As
other examples to test the detector, various
different organic conductors was measured. We can get good lattice parameters.
Now we are trying to do structure analysis
for these complicated system.

Fig. 1. Upper: The picture of the 2D-PSD at the settlement procedure. Lower: Snapshot of diffrcationfrom NaCl.

Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 527

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JAEA-Review 2011-050

1-8-8
1-8-7
Neutron imaging measurement using newly developed inorganic gadolinium
scintillator
J. H. Kaneko 1), S. Satoh 2), J. Haruna 1), S. Saeki 1), S. Kawamura 1), Y. Ohtake 3), M.
Furusaka 1), Y. Kiyanagi 1)1) Hokkaido University, 2) KEK, 3) RIKEN
1.

Introduction

To improve experimental efﬁciency, neutron imaging measurement using a newly
developed inorganic gadolinium scintillator was carried out. Cerium doped gadolinium pyrosilicate, i.e., GPS:Ce scintillator
has been developed by Hokkaido University. This scintillator has two times light
output higher than that of GSO scintillator;
in addition, it has fast decay time of 50 to 60
ns. Several types of GPS scintillator plates
were examined with combination of a position sensitive photo multiplier tube in theULS.

was obtained successfully. Detection efﬁciency of 70% was conﬁrmed by comparison between a Li glass scintillator. As future work, a uniform GPS scintillator plateshould be developed for higher spatial resolution in neutron imaging.

2. Experimental
Polycrystalline GPS scintillator was grownby ﬂoating zone melting method. The GPS
scintillator was grinded down and thenﬁxed by several substrates by adhesive.
Some of them were polished by mechanical way. Larger size of fabricated GPS scintillator plate was approximately 3 cm in diameter and 120 micrometer in thickness.
A special circuit developed in KEK for a
GPS scintillator was used. Figure 1 shows
schematic drawing of the detection system.

Fig. 1.

3. Experimental results
Figure 2 shows an example of pulse height
distribution from a charge sensitive preampliﬁer. Peaks caused by 33 keV internalconversion electrons and 77 keV that was
sum of 33 keV internal conversion electron and 44 keV characteristics X-ray wereclearly observed. Figure 3 shows neutron
imaging of a character of kita madeof cadmium plate. Although there was nothigh uniformity of scintillator, ﬁne image
Activity Report on Neutron Scattering Research: Experimental Reports 15 (2008)
Report Number: 663

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JAEA-Review 2011-050

1-8-9
Performance Test of Neutron Detector forEngineering Diﬀractometer in J-PARC
K. Sakasai, T. Nakamura, S. Harjo, A. Moriai, M. Katagiri,
K. Soyama, S. Satoh1 , E. Shooneveld2 , and N. Rhodes2
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195
Institute of Materials Structure Science, KEK,Tsukuba, 305-0801
2
ISIS Science Diﬀraction and Muon Division, RAL, Didcot, OX11 0QX, UK
1

Ihkl (θ) = K · J · A(θ, λ)L(θ)|Fhkl |2 ,where K is constant that is dependent on theexperimental conﬁguration, J is a multiplicity factor, A(θ,λ)is an absorption factor, L(θ)
原子炉：JRR-3

装置：MUSASI(T2-3)

is a Lorentz factor, and Fhkl is a structure
factor. Table 1 summarizes the results. The
estimated lattice spacings agreed very well tothe values by Harjo et al. 1)
In summary, the lattice spacing of a sample was well determined. New detectors thatmeet the actual requirements, e.g., a sensitive area of 196 mm × 1,000 mm and the secondary ﬂight path of 2.0 m, are now underconstruction for ﬁrst commissioning in 2008.
References
1) S. Harjo et al. :“Residual Thermal Phase Stressesin α-γ Fe-Cr-Ni Alloys Measured by a Neutron
Diﬀraction Time-of-Flight Method”, Mat. Trans.,
43, 1696(2002).

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A prototype linear scintillation neutron detector originally developed in RAL was fabricated for the engineering diﬀractometer in
J-PARC. In this paper, some results of theperformance test of the detector is described.
The fabricated detector was designed tohave a small detection pixel with a spatial resolution of 3 mm. The detector had 120 pixels to establish a large neutron sensitive area.
Scattered neutrons were detected based on a
nuclear reaction of 6 Li(n,α) in ZnS/LiF scintillators in the pixel. Incident neutron position was determined by a 2 Cn coding method.
The applied voltages of PMTs are individually set to have a gain of 3 x 107 . The
Si monochrometer was used for generation of
2.2 Å-neutrons. After comﬁrmation of fundamental performances such as output linearity, demonstration experiments for neutron
diﬀraction were carried out. In the experiment, a two-phase iron sample that has bothα-Fe and γ-Fe phases was used. Nickel powder and silicon powder were also used as reference sample.
Figure 1 shows neutron diﬀraction patternof the two-phase sample after calibration of
scattering angle using results of nickel andsilicon powders. After determination of eachscattering angle in the ﬁgure by Gaussian ﬁtting method, lattice spacings of α-Fe and γFe in the sample were determined according
to an equation of neutron scattering intensity
Ihkl (θ):

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$QJOHT GHJUHHFigure 1: Neutron diﬀraction pattern of the two-phasesample.

Table 1: Estimated lattice spacing (Å)

Phase
γ-Fe
α-Fe

This work
3.593
2.860

Harjo et al.
3.594642.87084

分野：中性子散乱（装置）㻙㻌 㻞㻥㻤㻌㻙

Diﬀ.(%)-0.05324-0.39245

JAEA-Review 2011-050

1-8-10Development of 3 He PSDs and Related Electronics for New Spectrometers in
J-PARC
K. Nakajima1 , T. Yokoo1,2 , S. Satoh1,2 , K. Shibata1 , N. Takahashi1 , R. Kajimoto1 ,T. Nakatani1 , Y. Inamura1 , N. Kaneko1,2 , Y. Yasu3 , K. Nakayoshi3 , E. Inoue3 , H. Sendai3
and M. Arai1
1

Neutron Science Section, MLF Division, J-PARC Center
Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK)3
Institute of Particle and Nuclear Studies, High Energy Accelerator Research Organization (KEK)
2

Various novel types of 3 He position sensitive detectors (PSDs) and related data acquisition electronics (DAQ) including software,
which are planed to be used at new spectrometers in J-PARC, have been tested at
MUSASI port. Since the detector is one of
the most important key components, it is indispensable to evaluate the feasibility and theperformance of these new detectors and related electronics prior to actual constructionof the instruments. We have continued theseeﬀorts from the beginning of our development work for J-PARC spectrometers and, in
JFY2007, mainly following items have been
subjected to be studied. 1. Performanceand feasibility studies of U-type detectors. 2.
Evaluation test of a new DAQ system using NEUNET. 3. Characterization studies of
PSDs. U-type detectors are sequentially coupled detectors. Since the connector is sharedby 2 pieces, we can reduce the installing space.
Such type of detectors will be employed at
Biomolecular Dynamics Spectrometer, DNAplanned for J-PARC. We have tested several
detectors from diﬀerent benders and have obtained enough performance at the ﬁnal moment. NEUNET is a new data processing
module for 3 He PSDs. This module equips
SiTCP developed by the University of Tokyoand can do high through put processing using
Ethernet. Practical trials were performed at
MUSASI port, and the expected performancehas been proven. These modules have been
already installed at several spectrometers in
J-PARC. We have also carried out characterization studies of PSDs to obtain data which
are necessary in operating existing PSDs anddesigning future purchasing detectors.
原子炉：JRR-3

装置：MUSASI(T2-3)

Figure 1: A prototype nunchakus-type detector (upper panel) and fully illuminated test setup, at whichfull part of the detector was illuminated by neutrons
scattered at a polyethylene block (lower panel).

Figure 2: A DAQ system with NEUNET modules (5black boards on the VME chassis) under the evaluation test at MUSASI port.

Figure 3: Obtained diﬀraction pattern from powder
Si by using prototype DAQ system with NEUNET.

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JAEA-Review 2011-050

1-8-11Development of Asymmetric Reﬂection-type Germanium Monochromatorfor Beam Flux Enhancement on HRPD
H. Yamauchi, Y. Ishii1 , N. Igawa, H. Fukazawa and W. Utsumi
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
1
Radiation Application Development Association, Tokai, Ibaraki 319-1106

The angle-dispersive neutron diﬀractometer, HRPD, installed at the research reactor JRR-3 in Japan Atomic Energy Agency
can provide high resolution powder diﬀraction data that meet the many users’ needs
until recently. On the other hand, the demand of high eﬃciency and high intensity inmeasurements is growing in late years. However, HRPD is not suitable for high intensity measurements because ﬁne Soller slittype collimators are placed in front of eachof the 64 detectors and ﬁxed in an angulardivergence of 6 , so that users cannot easilychoose the appropriate resolution for high efﬁcient measurements. In order to improve thesource intensity of the monochromatic neutron beam, the authors tried to develop asymmetric reﬂection-type monochromators usingmosaic germanium crystals.
According to theoretical considerations, theasymmetric reﬂection in compression geometry has an eﬀect on spatial condensation of
the neutron beam, which leads to the enhancement of the ﬂux density per unit area.
We used germanium single crystals as neutron monochromators, introducing the crystal mosaic of 20 in the horizontal direction
by hot pressing method. The mosaic crystals were cut at an angle of β = 40◦ relative

to the Ge(3 3 1) reﬂecting planes. Mosaicity
check and assembling of all mosaic crystals
were performed on TAS-2 and MUSASI-H.
Figure 1 shows the diﬀraction patterns of astandard powder sample (NIST 640c Si) measured by the new monochromator and existing
symmetric type one. The diﬀraction results
reveal that peak intensities by the asymmetricreﬂection-type monochromator are improved
1.2 times larger than those by the existing
symmetric type one, but integrated intensities
are almost comparable each other. For mosaic crystals, asymmetric reﬂections in compression geometry surely intensify the current
density, but reﬂectivity is always less thanthat in symmetric reﬂections, and thus the
suppression of the reﬂectivity just cancels out
the enhancement of the current density 1, 2) .
This is the reason why the asymmetric reﬂection has no practical eﬀect on the beam enhancement. In addition, it is reported thatbent crystals behave quite diﬀerently frommosaic crystals and show an eﬀective gain in
the neutron current density 2) .
References
1) S. A. Werner et al., Phys. Rev. 140, A675 (1965).
2) G. Albertini et al., Acta Cryst. A 33, 360 (1977).

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Figure 1: Diﬀraction patterns measured by the new monochromator and existing symmetric type one.

原子炉：JRR-3

装置：TAS-2(T2-4)

分野：中性子散乱（装置）㻙㻌 㻟㻜㻜㻌㻙

JAEA-Review 2011-050

1-8-12Development of High Quality Neutron Mirrors with Upgrading
Compact Cold Neutron Bender System II
I. Tamura, R. Maruyama1 , D. Yamazaki1 , K. Yamamoto, K. Nakamura and K. Soyama1
Nuclear Science Research Institute, JAEA, Tokai, Ibaraki 319-1195
1
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195

The compact cold neutron bender system
has been installed in JRR-3 beam hall to increase the number of beam ports with white
neutron beam. A transportation eﬃciency ofthe compact cold neutron bender system was
upgraded by using newly developed neutron
mirrors within the last couple of years. We
fabricated new high quality Ni/Ti multilayer
double sided neutron supermirrors with m=3
on silicon substrates in this year. These supermirrors was employed the ion beam sputtering technique. Large and thin silicon substrates whose size 40mm in width x 160 mm
in length and 0.2 mm in thickness were selected in order to improve the accuracy of
installation position. The neutron mirrors
were installed in the bender as curved neutron guides.
We report the neutron reﬂectivity of mirrors with the silicon substrates using cold neutron bender system.
The measurements of neutron reﬂectivityof newly produced neutron mirror have been
carried out at SUIREN1) at JRR-3 in theJapan Atomic Energy Agency. The incident
neutron wavelength was 3.93Å.
Neutron reﬂectivities of Ni/Ti supermirror
on the both side of the silicon substrate areshown in ﬁgure 1 and ﬁgure 2. Figure 1 shows
the neutron reﬂectivity of Ni/Ti supermirror
on one side of the silicon substrate and ﬁgure
2 shows the neutron reﬂectivity on the otherside of the same substrate. The reﬂectivities
at the eﬀective critical momentum transfer
were almost 0.9. The performances of the reﬂectivities of mirrors on one side of substrate
are almost same as that of the other side.
We succeeded in the manufacturing of thehigh reﬂectivity Ni/Ti multilayer neutron supermirrors with m=3 on both surfaces of thelarge and thin silicon substrate.
原子炉：JRR-3

装置：SUIREN(C2-2)

Figure 1: Neutron reﬂectivity on a front side of Ni/Ti
multilayer supermirror carried out at SUIREN.

Figure 2: Neutron reﬂectivity on a back side of Ni/Ti
multilayer supermirror carried out at SUIREN.

References
1) D. Yamazaki, et al. :“Development of a Neutron
Reﬂectometer SUIREN at JRR-3”, JAEA-Technology
2007-030 (2007).

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JAEA-Review 2011-050

1-8-13Development of High Reﬂectivity Neutron Supermirror
Using Ion Beam Sputtering Technique
R. Maruyama, D. Yamazaki, T. Ebisawa, and K. Soyama
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195

Although supermirrors with large criticalangle have been fabricated, the realization ofhigher reﬂectivity may be more important forneutron experiments. There is a techniqueof adding carbon atoms to the nickel layer
to suppress interface roughness that leads tohigher reﬂectivity 5) . We have also tested thistechnique and fabricated NiC/Ti supermirrors with m = 3 and 4. The measurementof neutron reﬂectivity was performed using
the JRR-3/SUIREN reﬂectometer at JAEA.
The incident average neutron wavelength was
0.39 nm with the resolution of 2.6% in the
FWHM. The divergent angle of the neutron
beam was less than 1 mrad. The reﬂectivityof those supermirrors at the critical angle was
0.88 and 0.82, respectively. The total numberof layers was 403 and 1201, respectively. Testfabrication of the NiC/Ti supermirror with
m = 6 was performed. The total number of
原子炉：JRR-3

装置：SUIREN(C2-2)

m= 1

2

3

4

0.4

0.6

0.8
-1
q / nm

5

6

1.0
0.8
Reflectivity

The development of high-performance neutron supermirrors with high reﬂectivity andlarge m, where m is the ratio of the eﬀective critical angle of the supermirror to thatof natural nickel, is important in neutron experiments, since they lead to a considerable
increase in available neutron intensity. We
have developed neutron supermirrors using
ion beam sputtering (IBS) since it enables
the production of layers with high density andsmall grain size 1, 2) . An IBS system with aneﬀective deposition area of 2,000 cm2 has been
installed at JAEA to produce neutron guides,
benders, and other optical devices based onsupermirrors for the new spallation neutron
source (Japan Proton Accelerator ResearchComplex, J-PARC). Ni/Ti supermirrors havebeen fabricated with large critical angles extending up to m = 3, 4, and 6.7 using the IBS
system. The neutron reﬂectivity of the supermirrors at the critical angle is 0.82, 0.66, and0.23, respectively 3, 4) .

0.6
0.4
0.2
0.0
0.2

1.0

1.2

1.4

Figure 1: Reﬂectivity proﬁles of NiC/Ti supermirrors
with m = 3, 4, and 6. Lines indicate the calculated
reﬂectivity proﬁles.

layers was 6003. Although an anomalous reduction in the reﬂectivity was observed, thecomparison of the measured reﬂectivity withthat calculated demonstrated that a NiC/Ti
supermirror with reﬂectivity of 0.40 at momentum transfer of 1.29 nm−1 (m = 6) can
be fabricated with a higher-precision deposition rate. By adopting NiC/Ti multilayers instead of Ni/Ti multilayers, higher reﬂectivity
has been realized 6) . We are therefore ready tocontribute to the J-PARC project by providing neutron guides, benders, and other opticaldevices based on supermirrors.
References
1) K. Soyama, W. Ishikawa, and K. Murakami, “J.
Phys. Chem. Solids” 60 1587(1999).
2) K. Soyama, H. Tsunoda, and K. Murakami, “Nucl.
Instrum. Methods Phys. Res. A” 529 73(2004).
3) R. Maruyama, D. Yamazaki, T. Ebisawa, M. Hino,and K. Soyama, “Physica B” 385-386 1256(2006).
4) R. Maruyama, D. Yamazaki, T. Ebisawa, M. Hino,and K. Soyama, “Thin Solid Films” 515 5704(2007).
5) J. Wood, “SPIE” 1738 22(1992).
6) R. Maruyama, D. Yamazaki, T. Ebisawa, and K.
Soyama, “Nucl. Instrm. Methods Phys. Res. A”
in print.

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JAEA-Review 2011-050

1-8-14
Neutron Reﬂectometer SUIREN: Status and Developments in 2007
D. Yamazaki, M. Takeda1 , R. Maruyama, M. Hino2 and K. Soyama
J-PARC Center, JAEA, Tokai-mura, Ibaraki 319-1195
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
2
Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494
1

At neutron reﬂectometer SUIREN (C2-2),
beam-line components has been developed formore eﬀective measurements since the start of
oparation in 2006. In 2007 following components were developed and installed:• new higher-harmonics ﬁlters (polarizing/
unpolarizing)(m∼4, Δd/d = 10%) coated on silicon wafersof 160 mm (L) × 60 mm (H) × 3 mm (T).
Polarization is ﬂipped by Mezei-type ﬂippers
and maintained with guide magnets which arecomposed of two parallel iron plates with four
ferrite brace between them. Figure 2 shows
measured polarization as a function of beamcollimation. It can be seen that polarization• a polarization analyzer

1• neutron spin ﬂippers and guide magnets

0.98

Polarization

0.96

The neutron wavelength have been changed
into 3.928 Å due to the installation of the newhigher-harmonics ﬁlters.
There are two higher-harmonics ﬁlters (apolarizing ﬁlter and unpolarizing one) both ofwhich reﬂect only nominal wavelength 3.928
Å while higher-harmonics neutrons are transmitted and absorbed as shown in Fig. 1. The
reﬂection angle of the 3.928Å neutrons is θ 
1.57deg, which corresponds to four times thecritical reﬂection angle of pure nickel (denoted
as m=4), for both ﬁlters.

0.94
0.92
0.9
0.88

S1w=0.4
S1w=1.0
S1w=2.0
S1w=4.0

0.86
0

0.05

0.1

0.15

0.2

0.25

0.3

0.35

0.4

Collimation Δθ (deg)Figure 2: Polarization as a function of beam collimation.

is no less than 0.95 even for loose collimations.
Neutron intensity is 7.6×104 n/cm2 /s undercollimation of Δθ = 0.08 deg. Resultant speciﬁcations of SUIREN are shown in Table 1.
Table 1: Speciﬁcations of SUIREN

λbeam size
Iunpol.
Ipol.
PbackgoundFigure 1: Filtering of higher-harmonics with wideband multilayer ﬁlter.

The unpolarizing ﬁlter is a NiC/Ti supermirror coated on a ﬂoat glass of 400 mm (L)× 100 mm (H) × 5 mm (T), and reﬂectivity
is 0.77. Neutron intensity is 1.8×104 n/cm2 /sunder collimation of Δθ = 0.08 deg.
The polarizing ﬁlter and the polarization
analyzer are Fe(Si)/Ge wideband-multilayer
原子炉：JRR-3

装置：SUIREN(C2-2)

3.928 Å (Δλ = 2.6%)
20 mmW × 80 mmH
1.8×104 n/cm2 /s (Δθ = 0.08◦ )7.6×103 n/cm2 /s (Δθ = 0.08◦ )> 0.95
4.5×10−3 n/s (shutter close)

SUIREN provided 67 days for the JAEA
common-use program and the MEXT trialuse program and were used for measurementon samples including magnetic thin ﬁlms andsolid-liquid interfaces.
分野：中性子散乱（装置）㻙㻌 㻟㻜㻟㻌㻙

JAEA-Review 2011-050

1-8-15Upgrading Compact Cold Neutron Bender System II
I. Tamura, R. Maruyama1 , D. Yamazaki1 , K. Yamamoto, K. Nakamura,
K. Aizawa1 and K. Soyama1
Nuclear Science Research Institute, JAEA, Tokai, Ibaraki 319-1195
1
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195

The compact cold neutron bender system
was used to branch oﬀ a cold neutron beamfrom a straight neutron guide to create additional guide end positions. The bender has
been installed in the C2 neutron guide at
JRR-3 beam hall and the bender provides newwhite cold neutron beam ports
However, the intensity of divided neutron
beams was too low to perform experiments effectively. Therefore, the neutron beam transportation eﬃciency of the cold neutron bender system was improved by using newly developed neutron mirrors.
Ni monolayer mirrors were replaced with
Ni/Ti multilayer supermirror on the curved
neutron guides section in the bender systembefore the JRR-3 operation in 2007.We report
the measured spectrum at the end of C2-3-3
beam port using a chopper spectrometer.
The neutron chopper has a 1400mm diameter disk, which has a slit of 10 mm width.The
disk of the neutron chopper operated with
5000rev/min rotation. A ﬂight path length

between the end of C2-3-3 beam port and the
chopper was 1.7m and a length between the
chopper and a detector was 1.3m.
The conversion factor from the time channel to the wavelength was calibrated on a
dip in the spectrum, which formed by an upstream monochromator in the neutron guide.
Figure 1 shows measured neutron spectraat the end of C2-3-3 beam port by the time-ofﬂight method before and after upgrade. The
characteristic wavelength of this beam port is
4.8 Å for after upgrade. The wavelength rangeof neutron beam was expanded and the intensity of neutron beam increased entire wavelength range. Measured neutron ﬂux at C23-3 beam port was 1.6×1011 (n/m2 s) by thegold foil activation method. The neutron ﬂux
incresed by 10 times after upgrade.

100

Intensity(cps)

10

1

0.1
before upgrade
after upgrade

0.01

0

2

4

6

8

10

12

14

Wavelength(Å)

Figure 1: Neutron spectra measured at C2-3-3 beam port before and after upgrade.

原子炉：JRR-3

装置：CHOP(C2-3-3)

分野：中性子散乱（装置）㻙㻌 㻟㻜㻠㻌㻙

JAEA-Review 2011-050

1-8-16
Neutron Detection by a MgB2 Transition Edge sensor
S. Okayasu1,2,5 , M. Katagiri1,5 , K. Houjo2,5 , Y. Morii1,5 , S. Miki3,5 , H. Shimakage3,5 , Z.
Wang3,5 and T. Ishida4,5
1

Quantum Beam Science Directorate , JAEA, Tokai, Ibaraki 319-1195
Advanced Science Research Center , JAEA, Tokai, Ibaraki 319-1195
3
KansaiAdvanced Research Center, NICT, Kobe, Hyogo 651-2492
3
Department of Physics and Electronics, Osaka Prefecture University, Sakai, Osaka 599-8531
3
JST-CREST, 5 Sanbancho, Chiyoda, Tokyo 102-0075
2

From the early stage of the discovery ofa new superconducting material MgB2 1) ,we have been investigating for neutron detection with a MgB2 transition edge sensor(TES) 2, 3) . For the purpose, we developed alow noise detecting system for neutron, andconﬁrmed the availability of the system byalpha ray from an americium-241 (241 Am)
source 4) . Using the system, we have achieved
the detection of a single neutron signal.
The 10 B atoms in MgB2 have an extremely
large cross section (3800 barns) with thermal
neutrons to be expressed as 10 B (n, α)7 Li withyielding a large nuclear energy of 2.31MeV.
The liberated energy destroys the superconducting state of MgB2 locally, and a hot spot
is generated in the sample. If the sample is
kept on the superconducting transition edge,a sharp resistance change due to the hot spot
can be observed.

were fabricated by the Kansai group in NiCT.
The sample preparations are described elsewhere 3, 5) . The 10 B-rich MgB2 samples (enriched 97% 10 B ) were fabricated to increase
the nuclear reaction.
A short meander line was used as shown inﬁg.1. A nuetron detected signal on the superconducting transition edge (Tc=26.3K) under constant current condition is also shownin ﬁg.2. The detected pulse width is about
10−8 second indicating fast responding time ofthe sensor.
References
1) J. Nakamatsu, et al.:“Nature”, 410, pp. 63 (2001).
2) K. Takahashi, et al.:“Physica C”, 392-396, pp.
1501 (2003).
3) S. Miki, et al.:“Nucl. Instr. Meth. A”, 529, pp.
405 (2004).
4) S. Okayasu, et al.:“Physica C”, in press.
5) H. Shimakage, et al.:“Physica C”, 392-396, pp.
1387 (2003).

Samples used in the detection experiments

Figure 1: MgB2 neutron detecting sensor

原子炉：JRR-3

装置：CHOP(C2-3-3)

Figure 2: Example of a detecting neutron
signal at 26.2K (I=-0.1mA).

分野：中性子散乱（装置）㻙㻌 㻟㻜㻡㻌㻙

JAEA-Review 2011-050

1-8-17
Application of a Magnetic Neutron Polarizing and Focusing Device to a
Focusing-Geometry Small-Angle Polarized Neutron Scattering Instrument
T. Oku, T. Shinohara, T. Kikuchi, Y. Oba, H. Iwase1 , S. Koizumi1 , J. Suzuki
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195

1

Quadrupole and sextupole magnets are
considered to be ideal neutron-polarizing andpolarized neutron-focusing devices, respectively, since no materials are required to be
put on the beam axis so that the neutrons
are free from neutron scattering and absorption by materials 1, 2) . Therefore, we can construct an ideal focusing-geometry small-angle“polarized” neutron scattering instrument by
utilizing the quadrupole magnet as a neutron
polarizing device and the sextupole magnet
as a neutron focusing device. In this study,
we have installed the quadrupole magnet in
the focusing geometry small-angle neutron
scattering (FSANS) instrument SANS-J-II at
JRR-3, in which the sextupole magnet has
been already installed 3, 4) , and investigated
the instrument’s performance. By comparing the obtained results with those obtainedwith conventional magnetic super-mirror polarizers, we discuss the improvement of theperformance.
The instrumental setup is shown in Fig.1.
SANS-J-II is equipped with a magnetic neutron lens based on an extended Halbach-type
permanent magnet together with magnetic
Fe/Si supermirror polarizers P1 and P2 3, 4) .
The polarization eﬃciencies of P1 and P2 are∼ 0.96 and ∼ 0.99, respectively 3) . The

quadrupole magnet is the Halbach-type permanent quadrupole magnet with an aperturesize of 5 mm in diameter and a length of 600
mm. The magnetic ﬁeld gradient ∂ |B| /∂r =791.9 ± 8.3 Tm−1 is generated inside the magnet. In the aperture of the quadrupole magnet, positive polarity neutrons are conﬁned
around the magnet center axis, but negative
polarity neutrons are accelerated away fromthe magnet center axis due to the magnetic
ﬁeld gradient. Therefore, a Cd slit with a 2mm-φ pinhole (Slit2) is attached at the endof the magnet. Then only the positive polarity neutrons can pass through the quadrupole
magnet aperture in this experimental condition. The neutrons are focused on the surface of the 2d-position-sensitive scintillation
detector (2d-PSD) and the neutron intensity
distributions are measured by the 2d-PSD.
Figs. 2 (a) and (b) show the radial distributions of the averaged intensity normalized by
the measuring time and the peak-height intensities, Ipeak , respectively. It is consideredthat the diﬀerence in the peak height of theintensity normalized by time is mainly causedby the diﬀerence in the neutron transmission property of the polarizing devices (Fig.
2(a)). Since P2 has a neutron transmission

Lmag = 1200

L1 = 7810

Al-window
Translation stage

150

L2= 10690

P1
1090
Vacuum chamber

Slit1
Neutronbeam

Spin flipper(SF)
SC1
2 mm - slit
(Slit2 )Ls= 9600

SC2

Sample
table

2500

V

Quadrupole magnet(Q-mag)

SC2

P2

Slit3
2

(20x20mm )Slit4

Solenoid CoilSolenoid coils
Magnetic neutron lensFigure 1: Experimental setup of SANS-J-II.

原子炉：JRR-3

装置：NOP(C3-1-2-1)

2d-PSD
Vacuum chamber(20x20mm 2)

分野：中性子散乱（装置）㻙㻌 㻟㻜㻢㻌㻙

Unit : mm

Intensity / Time [n/sr/sec]

JAEA-Review 2011-050

10

8

10

7

10

6

10

5

10

4

10

3

10

2

10

1

10

0

peak height ratio = 2.0(a)peak height ratio = 2.8

2

Slit1=1 x 1 mm
Quadrupole magnet
P1
P2

(b)

Intensity / I peak

-1

10

-2

10

Flat background

Peak broadening

-3

10

-4

10

-5

10

-6

10

2

Slit1=1 x 1 mm
Quadrupole magnet
P1
P2

-7

10

4

6 8

1

2

4

6 8

10

2

r [mm]
4

6 8

-4

10

2

4
-1

6 8

-3

2

10

q [Å ]

Figure 2: The radial averages of the intensity distributions. The intensities are normalized by (a) the measuring time and (b) the peak-height intensities Ipeak .
r is the distance from the peak center.

Tunpol ∼ 0.22 for unpolarized neutrons with
λ = 6.5Å 3) , the neutron transmissions of thequadrupole magnet and P1 are estimated to
be Tunpol ∼ 0.44 and Tunpol ∼ 0.16, respectively. Since the quadrupole magnet has very
high polarization eﬃciency P >∼ 0.99 and includes no materials which absorb and scatter
neutrons on the beam axis of the quadrupole
magnet, such a higher neutron transmission
can be obtained. In the case of using P1, a ﬂatbackground intensity region was observed asindicated in Fig. 2 (b). This background intensity is created by the negative polarity neutrons, because they are defocused by the magnetic neutron lens and spread over the detector homogeneously. On the other hand, sucha ﬂat background region was not observed in
the cases of using P2 and the quadrupole magnet with the higher polarizing eﬃciencies. In
Fig. 2 (b), relatively large peak broadeningof the intensity proﬁles was observed for P1
and P2 by comparing with the proﬁle for thequadrupole magnet. The peak broadenings
is considered to be the result of the neutron
scattering from the mirror materials of theP1 and P2 and/or the neutron reﬂection on
the Ni-side walls of the P2 3) . As the results of this study, the excellent performanceof the quadrupole magnet as the neutronpolarizing device based on its characteristics
such as high neutron transmission and highpolarization eﬃciency was demonstrated in
the application to the FSANS instrument using the magnetic neutron lens. The weak aspect of the quadrupole magnet based polarizer is its small opening aperture, which is
required to realize a suﬃciently strong magnetic ﬁeld gradient for the application. If theeﬀective aperture of the quadrupole magnet
is enlarged with keeping its polarizing powerby employing an extended-Halbach circuit ora superconducting magnet, the performanceof the FSANS instrument would be further
improved and another kind of its applicationsuch as a highly eﬃcient polarized-neutrontransporting guide would be expected.
In summary, we conclude that the FSANS
setup which is composed of the magnetic neutron lens and the neutron-polarizing device
based on the quadrupole magnet is considered to be suit for small-angle polarized neutron scattering measurements with high angular resolution.
References
1) H.M. Shimizu, et al. :“NIM-A”, 430, pp. 423-434(1999).
2) T. Oku, et al. :“Physica B”, 397, pp. 188-191(2007).
3) T. Oku, et al. :“J. Appl. Cryst.”, 40, pp. s408s413 (2007).
4) S. Koizumi, et al. : “J. Appl. Cryst.”, 40, pp.
s474-s479 (2007).

㻙㻌 㻟㻜㻣㻌㻙

1-8-17

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JAEA-Review 2011-050
















1.  ਛᕈሶᢔੂ 9 ⿥વዉ⃻⽎ 


1. Neutron Scattering



























㻙㻌 㻟㻜㻥㻌㻙

9)Superconductivity

This is a blank page.

JAEA-Review 2011-050

1-9-1
Emergence of Magnetic Modulations in the Overdoped Phase of Bi2201
by Fe Doping
H. Hiraka, S. Wakimoto1 , M. Takeda1 , K. Kakurai1 , and K. Yamada2
1

IMR, Tohoku University, Sendai, Miyagi 980-8577
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
2
AIMR(WPI), Tohoku University, Sendai, Miyagi 980-8577

Inelastic neutron scattering studies revealed that the so-called “hourglass-like”
magnetic-dispersion relation commonly exists
in high-Tc cuprates 1–3) , thus indicating themagnetic interaction as a prime candidateof pairing mechanism. However, no magnetic cross section has been ever reported in
Bi2 Sr2 CuO6+δ (Bi2201), which is one of themost typical cuprate superconductors. In order to resolve this puzzle, we grew large single crystals of Fe and Pb co-doped Bi2201 forneutron scattering experiments. The Fe atom
is doped to enhance magnetic scattering, andthe hole density of current Pb-doped samples
was estimated to be p ∼ 0.25 from Tc of asgrown crystals before Fe doping. Recently,
by means of unpolarized neutron scattering,
we discovered diﬀuse incommensurate peaks
around (π, π) below Tneu ∼ 30 K using a 9%Fe doped single crystal. Unexpectedly, the incommensurability reaches to δ ∼ 0.20, which
is much larger than that of magnetic modulations in La214 (δ max ≈ 0.13) 4) . Further,
the diﬀuse-peak width is very broad in the(h, k, 0)ort scattering plane, corresponding toa short correlation length of 1/κ < 10 Å on
the CuO2 plane. Prior to further inspection,
it is required to conﬁrm its origin of this intriguing cross section at ﬁrst.

trum at 3 K proves that the incommensurate cross section is magnetic in origin. Thisconsequence is also supported by the disappearance at high temperature (> Tneu ). The
emergence of the incommensurate-peak pattern strongly suggests incommensurate magnetic correlations underlying in the Cu spin
system. Now, we started searching for the“hourglass-like” magnetic excitations by unpolarized neutron scattering.

Polarized neutron experiments were carried out on the TAS-1 at JRR-3 using thesame 9%-Fe doped single crystal. A Heusler
monochromator and an analyzer were used
to generate spin polarized neutrons with energy of 14.7 meV. The plate-like sample with
5×2×30 mm3 in size was set to scan in the(h, k, 0)ort scattering plane. Figure 1 showspolarized neutron data under a spin-ﬂip modewith horizontal ﬁeld parallel to the scattering vector. The low-temperature Q spec-

Figure 1: Polarized neutron data under the spin-ﬂip
mode with horizontal ﬁeld of 10 Oe. The inset shows
the scan trajectory through incommensurate peaks.

原子炉：JRR-3

装置：TAS-1(2G)

Polarized neutron, Horizontal field & Spin flip
Bi1.75Pb0.35Sr1.90Cu0.91Fe0.09O6+δ , as-grown(h, k, 0)ort , TAS-1, 14.7Ef, B-80'-S-80'-B
ω = 0 meVk

< Counts / ~40 min >

400

0

1

h

3K

300

200

120 K
100
-0.5

0

1-2-500.5(0.8, k, 0)

References
1) J.M. Tranquada et al., Nature 429, 524 (2004).
2) C. Stock et al., Phys. Rev. B 71, 024522 (2005).
3) B. Fauque et al., Phys. Rev. B 76, 214512 (2007).
4) K. Yamada et al., Phys. Rev. B 57, 6165 (1998).

分野：中性子散乱（超伝導）㻙㻌 㻟㻝㻝㻌㻙

JAEA-Review 2011-050

1-9-2
Peculiar Field Response of Antiferromagnetism in non-centrosymmetricheavy fermion superconductor CePt3 Si
K. Kaneko1 , N. Metoki1 , T. Takeuchi2 , T.D. Matsuda1 , Y. Haga1 ,R. Settai3 , Y. Ōnuki1,3
Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Naka, Ibaraki 319-1195
2
Low Temperature Center, Osaka University, Toyonaka 560-0043
3
Graduate School of Science, Osaka University, Toyonaka 560-0043

Three single crystalline samples of CePt3 Si
with the total mass of 2 grams were assembled within 1 degree and used for the present
study. Neutron diﬀraction experiments werecarried out on the cold triple-axis spectrometer LTAS installed in the guide hall. A incident wavevector of 1.5 Å−1 was employed,
and the cooled Be ﬁlter was put on ki in order to remove the higher order contamination. Horizontal ﬁeld magnet was used together with the hand-made dilution insert.
Figure 1 shows the 0 0 1/2 reﬂection intensity at 0.56 K as a function of external mag原子炉：JRR-3

装置：LTAS(C2-1)

63

Non-centrosymmetric heavy fermion superconductor CePt3 Si attracts a surge of interest since novel superconducting properties are
expected under a of inversion symmetry in a
crystal structure1) . CePt3 Si exhibits an antiferromagnetic (AFM) transition at TN =2.2 K,
which is followed by a superconducting transition at Tsc ∼0.45 K. In addition to the lackof inversion symmetry, the characteristics ofthe superconductivity in CePt3 Si are its coexistence with the long range AFM order2) .
We clariﬁed that the AFM order in CePt3 Si
is commensurate with q =(0 0 1/2) in which
reduced magnetic moment of 0.17 μB orientsparallel to 1002) . The AFM reﬂection does
not exhibit an anomaly on passing throughTsc and persists down to the lowest temperature. In contrast to the temperature variation, AFM reﬂection intensity shows a peculiar response against external magnetic ﬁeld;
the intensity of AFM reﬂection is enhancedwith applying ﬁelds, especially for H [0 0 1]3) .
This response is opposite to an usual antiferromagnet. Since these measurements havebeen carried out only down to 1.5 K so far, we
tried to extend the scan range to lower temperature in the present study.

10 counts / 60 sec

1

CePt3Si As#3
( 0 0 1/2 )0.56 K

4

2

background

0
0

1

2

3

4

5

 H ( T )Figure 1: The 0 0 1/2 antiferromagnetic reﬂection intensity of CePt3 Si at 0.56 K as a function of external
magnetic ﬁeld for H [0 0 1].

netic ﬁeld applied for H [0 0 1]. The AFM
intensity shows strong enhancement with applying ﬁelds at 0.56 K well below TN . The intensity at 5 T becomes 4 times stronger thanthat at zero ﬁeld and keeps increasing evenaround 5 T. This indicates that the AFM ordered moment becomes double at 5 T. Furthermore, the ﬁeld dependence of intensity
shows an inﬂection point around 4 T, whichmatches the reported additional boundary in
the H-T phase diagram4) . The origin of both
the AFM moment enhancement and the additional phase boundary are unclear at present.
Inelastic scattering experiments under ﬁelds
are in progress in order to clarify these phenomena.
References
1) E. Bauer et al., Phys. Rev. Lett. 92, 027003 (2004).
2) N. Metoki et al., J. Phys.: Condens. Matter 16,
L207 (2004).
3) K. Kaneko et al., J. Phys. Soc. Jpn. 75, Suppl.
pp. 177 (2006).
4) T. Takeuchi et al., J. Phys. Soc. Jpn., 76, 014702(2007).

分野：中性子散乱（超伝導）㻙㻌 㻟㻝㻞㻌㻙

JAEA-Review 2011-050
















1.  ਛᕈሶᢔੂ 10 ᱷ⇐ᔕജ 


1. Neutron Scattering㻙㻌 㻟㻝㻟㻌㻙

10 Residual StressThis is a blank page.

JAEA-Review 2011-050

1-10-1
Strain Evaluation of Rebar in Reinforced Concrete Using Neutron Diﬀraction
M. Kanematsu, T. Noguchi1 , M. Yasuda2 and H. Suzuki3
1

Department of Architecture, Tokyo University of Science, Noda, Chiba 278-8510
Department of Architecture, University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113-8656
2
Toyo Construction Co., Ltd, Miura, Ibaraki 300-0424
3
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Reinforced concrete is known as the composite material of concrete and rebar, so thatthe stress balance between rebar and concrete is aﬀected by the bond condition between them. Therefore, it is very important
to know the strain distribution on the rebar
in the reinforced concrete in order to evaluate
the bond condition. In this study, we applied
neutron diﬀraction technique to measure thestrain distribution on the rebar in the reinforced concrete.
At ﬁrst, lattice strains of ferrite 110 reﬂection on the rebar was measured during
uniaxial tensile loading in order to verify
accuracy of the strain measurement of therebar covered by concrete. Lattice strains
were measured on the rebar with diameter of
18mm passed through the hole with diameter of 20mm machined in the rectangular concrete structure with the size of a×a×150mm(a=50mm and 70mm). Figure 1 shows theresult of change in diﬀraction angle with respect to the applied stresses. Average diﬀraction angles at some positions on the rebar
were plotted in this ﬁgure. Diﬀraction angles were plotted near the same line as thatof rebar without concrete regardless of sample conditions. Therefore, it was conﬁrmedthat eﬀects of concrete conditions i.e., sample
size and water content, on accuracy of strain
measurement on the rebar were negligible.
Secondly, strain distributions on the rebar in the reinforced concrete were measured
around cracks during tensile loading. Figure
2 shows the strain distributions on the rebar around cracks under applied stresses ofapproximately 150MPa and 300MPa as well
as stress-free condition. Compressive residual strain can be observed in stress-free condition due to drying shrinkage. Strains trans原子炉：JRR-3

装置：RESA(T2-1)

ferred to the rebar were 60% to 80% of applied strains because of stress share with concrete. Moreover, scattering around cracks
were observed due to stress relaxation aroundcracks and also due to stress concentration
around rib. These results indicate that neutron diﬀraction technique probably enables tomeasure detailed strain distribution and toevaluate the damage region around cracks accurately.

Figure 1: Changes in diﬀraction angle with respect toapplied stress in each concrete sample and rebar only.

Figure 2: Strain distributions on the rebar aroundcracks in the reinforced concrete under tensile loading.

分野：中性子散乱（残留応力）㻙㻌 㻟㻝㻡㻌㻙

JAEA-Review 2011-050

1-10-2
Residual Stress and Deformation Behavior on Zr55 Al10 Ni5 Cu30
Bulk Metallic Glass Containing ZrC Particles
H. Suzuki, J. Saida1 and M. Imafuku2
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Center for Interdisciplinary Research, Tohoku University, Sendai 980-8578
2
Materials Characterization Center, NSTR, Futtsu, Chiba 293-0011

It has been developed that bulk metallic glasses containing hard particles or ﬁbers
exhibit higher strength and higher compressive plasticity as compared with monolithic
bulk metallic glasses 1) . In order to clarify the mechanism of these unique behavior, residual stress and deformation behaviorof Zr55 Al10 Ni5 Cu30 bulk metallic glass containing 10vol%ZrC particles (10%ZrC-BMG)
were evaluated using neutron diﬀraction technique.

strength on the 10vol%ZrC-BMG, reached
1785MPa in compression which is close
to the compressive strength, approximately
1.8GPa 1) , of the monolithic Zr55 Al10 Ni5 Cu30
bulk metallic glass. This is probably one of
the reasons why the compressive strength of
the bulk metallic glass reinforced by hard particles is higher than that of the monolithic
bulk metallic glass.

RESA diﬀractometer was utilized in thisstudy. At ﬁrst, residual stress and deformation behavior of ZrC particles, which are crystalline phase, were evaluated using neutron
diﬀraction, and then, those of the metallic
glass matrix were predicted by the composite
law in assumption of stress balance between
each phase.
Residual stresses in the ZrC phase and themetallic glass matrix were hydrostatic conditions of approximately 1.0GPa in compression and approximately 100MPa in tension,respectively. This relationship of residual
stresses between each phase to develop during cooling could be explained by mismatchof the thermal expansion coeﬃcients between
each phase.
Figure 1 shows the elastic deformation behavior under uniaxial tensile loading. Linear response in both phases can be observedin this ﬁgure, and the deformation behaviors
of each phase agreed well with those calculated by the Self-Consistent model. Figure
2 shows the compressive deformation behaviors of each phase up to 2.2GPa predicted by
the Self-Consistent model with considerationof the residual stresses in each phase. Phasestress of the metallic glass matrix at 2.0GPa of
applied stress, which is compressive fracture
原子炉：JRR-3

装置：RESA(T2-1)

Figure 1: Elastic deformation behaviors of each phase
under uniaxial tensile loading.

Figure 2: Compressive deformation behaviors predicted by the Self-Consistent model.

References
1) H. Kato et al, Scripta Mater., 43, 503(2000).

分野：中性子散乱（残留応力）㻙㻌 㻟㻝㻢㻌㻙

JAEA-Review 2011-050

1-10-3
Bulky Measurement of Gradient Texture of an IF Steel by Neutron Diﬀraction
P.G. Xu, Y. Tomota, H. Suzuki1 and S. Machiya1
Graduate School of Science and Engineering, Ibaraki University, Hitachi, Ibaraki, 316-8511
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

1. Introduction
As one of the factors inﬂuencing on the mechanical/physical properties of steels, texture
is usually measured by X-ray diﬀraction. The
texture is heterogeneous so that bulky texture
is determined by a serial sectioning method
etc., but there is a limitation of accuracy. Because neutron penetrates a bulk sample andhence it is hopeful to determine the bulky average in a gradient textured material. In thisstudy, 110, 200 and 211 pole ﬁgures of aninterstitial-free (IF) steel were measured byneutron diﬀraction with an angular dispersion
method.
2. Experimental Procedures
A 0.68mm-thick annealed IF steel containing
0.0018C-0.01Si-0.17Mn-0.013P0.006S-0.01Cu- 0.01Ni-0.02Cr-0.003V-0.03Ti0.026Nb-0.033Alsolute-0.0014Ntotal (mass%)
was used. The 15×15mm sheets were stacked
up to be a cubic sample with the consistentrolling direction and the edges of the sheets
were adhered with a small amount of glue.
The 110, 200 and 211 pole ﬁgures were
measured with a neutron diﬀractometer,
RESA, at JAEA with a neutron wavelengthof 0.18nm, a 5mm×5mm slit for incident
beam and a 5mm collimator before PSD.

3. Results and Discussion
Figure 1 shows the orientation mapping
obtained by EBSD. As seen, microstructurechanges through the sheet thickness. Perfectpole ﬁgures were obtained by neutron diﬀraction and crystal orientation distribution function (ODF) was calculated as shown in Fig.
2. Compared with the X-ray textures and the
EBSD orientation mappings, the Gaussian integrated intensity obtained from each neutron
diﬀraction proﬁle can evaluate the bulk texture with a high accuracy.

Figure 2: ODF determined by neutron diﬀraction.

Figure 1: Crystal orientation mapping obtained by EBSD through the thickness direction (surface (left) tocenter).

原子炉：JRR-3

装置：RESA(T2-1)

分野：中性子散乱（残留応力）㻙㻌 㻟㻝㻣㻌㻙

JAEA-Review 2011-050

1-10-4
Engineering diﬀractometer ”RESA” and ”RESA-II”
H. Suzuki, T. Saito, S. Machiya, Y. Tsuchiya, A. Moriai, Y. Shimojo, K. Akita and Y. Morii
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Recently, the industrial users are interested
in using the neutron stress measurement for
ensuring the reliability of mechanical components, and the number of such users is
rapidly increasing each year. As a result of
that, measurement eﬃciency had to be improved by modifying the RESA diﬀractometer in order to satisfy many needs and the expectations from industrial users. Figure 1(a)shows the upgraded engineering diﬀratometer, RESA. Wavelength can be selected fromapproximately 0.16 nm to 0.21 nm by using
asymmetrical bent crystal silicon monochromator. Large scale XYZ goniometer with thesize of 1000 mm x 1000 mm top plate and theload capacity of 800 kgf was developed. Two
axis diﬀractometer was replaced to low heighttype to get about 400 mm distance in maximum from beam height to top surface of the
XYZ goniometer. The one-dimensional position sensitive detector (PSD) with 100 mm x
100 mm active area is installed for improving eﬃciency of the neutron detection, andthe radial collimator system can be set before PSD to deﬁne the gauge volume (0.5mm, 1.0 mm, 2.0 mm, 3.0 mm and 5.0 mm).
These upgrades related to the detector willachieve single-digit measurement eﬃciency increase compared with RESA before upgrades.
Sample oscillation function was added for allowing the stress measurement of large grain
polycrystalline samples. These improvementsof RESA would bring the further promotion ofindustrial use of neutron stress measurement.
As described above, the number of RESA
users is rapidly increasing each year. Since
there was only one diﬀratometer for engineering application, almost users could not
get enough beam time to achieve their experiment. Therefore, the 2nd engineering
diﬀratometer, called RESA-II, was installedat T2-3-2 beam port in the guide hall of the
JRR-3, as shown in Fig. 1(b). Relatively
原子炉：JRR-3

small type diﬀractometer was installed on thesteel board with the size of approximately
1500 mm x 2000 mm. PSD with 50 mm x 100
mm active area is utilized, and relationshipof slits set before and after sample can deﬁne the gauge volume. Wavelength of RESAII is ﬁxed at approximately 0.21 nm. Small
type of XYZ goniometer with the size of 300
mm x 300 mm top plate and load capacityof approximately 20 kgf can be installed, andthe distance from beam height to top surfaceof the XYZ goniometer is approximately 245
mm in maximum. In addition, the quarter
type Euler cradle can be installed. Operationof RESA-II is the same as that of RESA, so it
is convenient for RESA users. Measurement
eﬃciency is smaller than that of RESA, however, RESA-II can be suﬃciently applied to
not only residual stress measurement of small
mechanical components but also microstructural analysis of deformed materials.

Figure 1: Upgraded RESA and 2nd engineering
diﬀractometer RESA-II.

装置：RESA(T2-1), RESA-II(T2-3-2)

㻙㻌 㻟㻝㻤㻌㻙

分野：中性子散乱（残留応力）

JAEA-Review 2011-050
















2.  ਛᕈሶ࡜ࠫࠝࠣ࡜ࡈࠖ 

2. Neutron Radiography㻙㻌 㻟㻝㻥㻌㻙This is a blank page.

JAEA-Review 2011-050

2-1
Fundamental Experiments for the Development of an Advanced Neutron
Tomography
M. Kureta
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195

1. Introduction
Fundamental high-frame-rate neutron radiography and neutron tomography experiments
were performed in order to develop the highframe-rate (HFR) neutron tomography technique which is an advanced neutron visualization and measurement technique. Merit of the
HFR neutron tomography techniques are onethat neutron irradiation time becomes short,and second that its makes 4D visualizationand measurement possible. The experiments
were carried out in the TNRF of JRR-3.
2. Experimental Setup
High-frame-rate video camera with image intensiﬁer system are used instead of the cooled
CCD camera system. And the test object was
rotated quickly on the turn table. Many kindsof test object were used for the developmentof the HFR neutron tomography techniquesuch as a toy boat, bubbling water can, sandglass etc. Recording frame rate and rotating
speed are changed as a test parameter. Neutron beam shutter is opened very short timecompared with the CCD camera system suchas 3 sec. There for, activation of the test object becomes very small. Nominal recording
image size was 512x512 pixel, and the depth
resolution was 10bit (1024 grayscale).

JIPANG. Instantaneous 3D CT value distribution was successfully calculated.
4. Summary
For the development of an advanced neutron
tomography technique, the HFR neutron tomography experiments has been carried out
in the TNRF-2 of the JRR-3. Also, dataprocessing code and visualization software are
improved to correspond to the HFR neutron
tomography. Consecutive instantaneous 3DCT value distribution could be calculated after the experiments. The development has
been continued. At this moment, as this technique will be got a patent, detailed results will
be opened after the patent is accepted.

3. Experimental Results
Consecutive images of the neutron radiography were recorded while the test object is rotated. For example, 1000 consecutive and 360
degree revolved images are recorded when the
1000fps and 1rps while 1sec. If the test object was moved while the recording, we canobserve the moving radiography image. Afterthe recording, image processing method andvisualization technique has been investigatedbased on the developed image data processing code NIPPON and visualization software
原子炉：JRR-3

装置：NRF(7R, C2-3-3-1)

㻙㻌 㻟㻞㻝㻌㻙

分野：中性子ラジオグラフィー（熱水力）JAEA-Review 2011-050

2-2Development of an Ultra-High-Speed Scanning Neutron
Tomography System for High-Quality and Four-Dimensional
Visualizations
M. Kureta, H. Iikura1
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

A new neutron tomography imaging system was developed in order to realize
a high-quality three-dimensional (3D) and
four-dimensional (4D) visualizations by fusing high-frame-rate neutron radiography andcomputed tomography (CT) techniques. Fundamental idea (patent-JP2008-4247) is thatthe object is revolved with high rotating speed
ranging from 0.1 to 10 rps and the neutron
radiography images are recorded with a highspeed video camera and an image intensiﬁer,
and then the consecutive images are processedby 3D CT technique. When we need to visualize the time change of the 3D distribution, 3D CT data processing is continued ontime axis in increments of more than one time
step. Fundamental tests were carried out at
the TNRF in the research reactor JRR-3 of
JAEA to proof this new technique. Figure 1
shows an outside view of the 3D CT data (Fig.
1(a)) and the cut view (Fig. 1(b)). Object rotating speed for Fig. 1 condition was 1 rps,
recording speed was 2,000 fps and projection
number was 2,000 / 360 degree. We could get
the ﬁne 3D distribution of the CT values as

Figure 1: 3D-CT sample image (2,000 projection numbers; 2,000 fps; 1 revolution per second).

shown in Fig. 1. 4D CT images of the sample (two sandglasses) were shown in Fig. 2.
Object rotating speed was 0.25 rps, recording
speed was 60 fps and projection number was
240 / 360 degree. These imaging conditions
should be regulated depending on the researchtarget. This new technique has also an advantage to reduce radio- activation of the object
materials remarkably.

Figure 2: 4D-CT sample image (240 projection numbers; 60 fps; 0.25 revolution per second).

原子炉：JRR-3
燃料・材料）

装置：NRF(7R, C2-3-3-1)

㻙㻌 㻟㻞㻞㻌㻙

分野：中性子ラジオグラフィー（原子炉用JAEA-Review 2011-050

2-3
JRR-3M ⇕୰ᛶᏊࢆ฼⏝ࡋࡓΰ┦ὶࡢືែィἲࡢ㧗ᗘ໬-IIDevelopment of Measurements for Multiphase Flow Dynamics -II
by Using Neutron Beam of JRR-3M
ி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤ ୕ᓥ ჆୍㑻

1. ◊✲┠ⓗἛ㦐ࡸจ⦰ࢆక࠺ΰ┦ὶࡣࠊከࡃࡢືຊࣉࣛࣥࢺࠊ
໬Ꮫࣉࣛࣥࢺ࠾ࡼࡧ✵ㄪ࣭෭෾⿦⨨࡟㛵ಀࡋࠊࡇࢀ
ࡽࡢᶵჾࡢ᭱㐺タィࢆ⾜࠺ୖ࡛ᴟࡵ࡚㔜せ࡛࠶ࡿࠋ㏆ᖺࠊẼᾮ஧┦ὶࡸᅛᾮ஧┦ὶ࡟㛵ࡋ࡚ᵝࠎ࡞ᩘ್ゎᯒᡭἲࡀⓎ㐩ࡋࠊゎᯒᑐ㇟࡟ࡼࡗ࡚ࡣ⢭ᗘࡢ㧗࠸ண ࡀྍ⬟࡜࡞ࡗ࡚ࡁ࡚࠸ࡿࡀࠊ㧗ࣞ࢖ࣀࣝࢬᩘὶ
ࢀࡸ┦ኚ໬ࢆక࠺ΰ┦ὶ࡞࡝࡟ࡘ࠸࡚ࡣᚲࡎࡋࡶ⌮ゎࡣ༑ศ࡛ࡣ࡞ࡃࠊࡉࡽ࡟᳨ウࢆ⾜࠺ᚲせࡀ࠶ࡿࠋ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ࡣ X ⥺㸦࠶ࡿ࠸ࡣ & ⥺㸧ࣛࢪ࢜ࢢࣛࣇ࢕࡜┦⿵ⓗ࡞ᛶ㉁ࢆ᭷ࡋࠊΰ┦ὶィ ࡟㈗㔜࡞᝟ሗࢆᥦ౪ࡍࡿ᭷ຊ࡞ࢶ࣮ࣝࡢ୍ࡘ࡛࠶ࡿࠋ
ࡋ࠿ࡋࠊ᫬㛫ᖹᆒࢆᑐ㇟࡜ࡋࡓ࣎࢖ࢻ⋡ィ ࡸ CTゎᯒࡢᢏ⾡ࡣ࡯ࡰ☜❧ࡋ࡚࠸ࡿࡶࡢࡢࠊΰ┦ὶࡢືែィ ἲ࡟⮳ࡗ࡚ࡣᩘከࡃࡢㄢ㢟ࡀṧࡉࢀ࡚࠸ࡿࠋ
㧗㏿ᗘ࡛ືែࢆィ ࡍࡿ㝿ࡢㄢ㢟ࡢ୍ࡘࡣࠊ⏬㉁ࡢຎ໬࡛࠶ࡿࠋࡇࢀࡣ୰ᛶᏊࡢィᩘㄗᕪ࡜᧜ീ⣔ࡢࣀ࢖ࢬ࡟㉳ᅉࡍࡿࡀࠊࡶࡋ୰ᛶᏊ᮰ࡢቑ኱ࡀᮃࡵ࡞
࠸࡜ࡍࢀࡤ᧜ീ⣔ࢆᨵⰋࡍࡿࡋ࠿᪉ἲࡣṧࡉࢀ࡚࠸࡞࠸ࠋி㒔኱Ꮫࡢ◊✲ࢢ࣮ࣝࣉ࡛ࡣࠊࡇࢀࡲ࡛㧗ឤᗘ࢖࣓࣮ࢪ࣭࢖ࣥࢸࣥࢩࣇ࢓࢖࢔ࡢග㟁㠃࡟୰ᛶᏊ⏝⺯ගࢥࣥࣂ࣮ࢱ࡜┦ᛶࡢⰋ࠸༙ᑟయග㟁㠃
㸦GaAsP㸧ࢆ㑅ᢥࡋࠊ㧗ゎീᗘ㧗㏿ᗘ࣓࢝ࣛ࡜⤌ࡳྜࢃࡏࡿࡇ࡜࡛ࣀ࢖ࢬࡢపῶࢆ⾜ࡗ࡚ࡁࡓ 1)ࠋࡋ࠿
ࡋࠊ⺯ගࢥࣥࣂ࣮ࢱࢆ⏝࠸࡚㧗ឤᗘ࣭㧗ゎീᗘࢆ⌧ᅾ௨ୖࡢ㧗࠸࡛ࣞ࣋ࣝ୧❧ࡉࡏࡿࡇ࡜ࡣᴟࡵ࡚ᅔ㞴࡛࠶ࡾࠊ௒ᚋࡣ᧜ീ⣔ࡢ㔞Ꮚຠ⋡ࢆࡉࡽ࡟ྥୖࡉࡏ
ࡿࡓࡵ࡟ࡣࠊ୰ᛶᏊ࢖࣓࣮ࢪ࣭࢖ࣥࢸࣥࢩࣇ࢓࢖࢔
࡞࡝ࡢ㛤Ⓨࡀᚲせ࡛࠶ࢁ࠺ 2, 3)ࠋ
ࡶ࠺୍ࡘࡢㄢ㢟࡜ࡋ࡚ࡣࠊᚓࡽࢀࡓ⏬ീ࠿ࡽΰ┦ὶࡢ⌮ゎ࡟ᑐࡋ࡚᭷┈࡞᝟ሗࢆᢳฟࡍࡿィ ฎ⌮ᡭἲࢆ㛤Ⓨࡍࡿࡇ࡜࡛࠶ࡿࠋࡇࢀࡲ࡛ࡢඹྠ฼⏝࡛ࡣ୺࡟୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕㧗㏿ᗘ᧜ീἲ࡜
PIV(Particle Image Velocimetry) ࡸ PTV(Particle
Tracking Velocimetry)ࢆే⏝ࡋ࡚ࠊᾮయ㔠ᒓ஧┦ὶࡢᾮ┦㏿ᗘศᕸィ ἲࢆ㛤Ⓨࡋ࡚ࡁࡓ 4)ࠋࡋ࠿ࡋ࡞ࡀ
ࡽࠊࡇࢀࡲ࡛ࡢయ⣔ࡣࠊᛴ⃭࡞┦ኚ໬ࢆྵࡴయ⣔࡛ࡣ࡞࠿ࡗࡓࠋ
௒ᅇࡢඹྠ฼⏝࡛ࡣࠊ┦ኚ໬ࢆྵࡴᾮయ㔠ᒓὶࢆᑐ㇟࡜ࡋ࡚ᐇ㦂ࢆ⾜࠸ࠊᚓࡽࢀࡓ⏬ീ࠿ࡽ⇕ὶື◊✲࡟᭷⏝࡞≀⌮㔞ࢆ⟬ฟࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡋࡓࠋ2. ⁐⼥㔠ᒓ୰࡟࠾ࡅࡿᾮ⁲ࡢ┤᥋᥋ゐ⵨Ⓨ⌧㇟౛࠼ࡤࠊᾮయ㔠ᒓ෭༷㧗㏿ቑṪ⅔࡛ࢩࣅ࢔࢔ࢡࢩࢹࣥࢺࡀⓎ⏕ࡋࠊ⅔ᚰࡀ⁐⼥ࡋࡓሙྜ࡟ࡣ⇞ᩱ࡜ࢫࢸ࢕࣮ࣝ࠿ࡽ࡞ࡿἛ㦐ࣉ࣮ࣝࡀᙧᡂࡉࢀࡿࡇ࡜ࡀண
ࡉࢀ࡚࠸ࡿࠋࡇࡢሙྜࠊࢫࢸ࢕࣮ࣝࡢἛⅬࡀ⇞ᩱࡢ⼥Ⅼ࡜࡯ࡰ➼ࡋ࠸ࡓࡵ࡟ࠊ⁐⼥⇞ᩱ୰࡛ࠊᵓ㐀ᮦ࡛࠶ࡿࢫࢸ࢕࣮ࣝࡀἛ㦐ࡍࡿࠋࡇࡢἛ㦐஧┦ὶࡣᾮయ࡜Ẽయࡢᐦᗘẚࡀ㏻ᖖࡢẼᾮ஧┦ὶ࡜ẚ㍑ࡋ࡚ 1᱆⛬ᗘ㧗ࡃࠊ㧗ᐦᗘẚࡢẼᾮ஧┦ὶࢆᙧᡂࡍࡿࠋࡇ
ࢀࡲ࡛ࠊி㒔኱Ꮫࡢࢢ࣮ࣝࣉ࡛ࡣࡇࡢ㧗ᐦẚẼᾮ஧┦ὶࡢ≉ᛶࢆゎ᫂ࡍࡿࡓࡵ࡟ᵝࠎ࡞ᐇ㦂ࢆ⾜ࡗ࡚ࡁࡓࠋࡋ࠿ࡋ࡞ࡀࡽࠊἛ㦐ࡢࢯ࣮ࢫ࡜࡞ࡿࢫࢸ࢕࣮ࣝ
ࡢἛ㦐㸭⵨Ⓨ⌧㇟࡟ࡣゝཬࡋ࡚࠸࡞࠸ࠋᮏ◊✲࡛ࡣࠊࡇࡢ㧗ᐦᗘẚయ⣔࡟࠾ࡅࡿ┤᥋᥋ゐ⵨Ⓨ⌧㇟ࢆᑐ㇟࡜ࡋ࡚ࠊ⁐⼥㔠ᒓ୰㸫Ỉࡢ┤᥋᥋ゐ⵨Ⓨ⌧㇟ࢆ࡜ࡾ࠶ࡆࡓ 5)ࠋ
ຍ⇕ࡉࢀࡓ⁐⼥㔠ᒓෆ࡟ᾮ⁲ࢆᄇᑕࡉࡏࡿ࡜ࠊᾮ
⁲ࡣ⁐⼥㔠ᒓෆ࡛⵨Ⓨࡋ࡞ࡀࡽ⁐⼥㔠ᒓ୰ࢆୖ᪼ࡍ
ࡿࠋࡇࡢሙྜࠊ஧┦ẼἻࡢయ✚ኚ໬ࢆ୰ᛶᏊࣛࢪ࢜
ࢢࣛࣇ࢕ࢆ⏝࠸࡚ィ ࡍࢀࡤ⵨Ⓨ㏿ᗘࡀ⟬ฟࡀྍ⬟࡛࠶ࡿࠋḟ࡟⏺㠃࡟࠾ࡅࡿ⇕ఏ㐩⋡ࢆ≉ᐃࡍࡿࡓࡵ
࡟ࡣ⏺㠃㠃✚ࢆồࡵࡿᚲせࡀ࠶ࡿࡀ⌫ᙧࢆ௬ᐃࡍࡿ
ࡇ࡜࡛⟬ฟࡀྍ⬟࡛࠶ࡿࠋࡋࡓࡀࡗ࡚ࠊᮏ◊✲࡛ࡣࠊࡲࡎࠊ⌫ᙧࢆ௬ᐃࡋ࡚ゎᯒࢆ⾜ࡗࡓࠋࡉࡽ࡟ࠊ༢୍
ᾮ⁲ࢆᄇᑕࡉࡏࡓሙྜ࡟ࡣࠊ㏻ᖖࡢẼᾮ஧┦ὶ࡜ྠᵝ࡟Ỉ࡜⵨Ẽ࠿ࡽ࡞ࡿ஧┦ẼἻࡣ⌫ᙧࡸᴃ෇ᙧࠊࡉ
ࡽ࡟ࡣ➟≧࡜ኚ໬ࡍࡿࠋከࡃࡢሙྜ࡟ࡣࡇࢀࡽࡢẼἻᙧ≧ࡣ Fig.1 ࡟♧ࡍࡼ࠺࡟ᅇ㌿ᑐ⛠య࡜࡞ࡿࡇ࡜
ࡀከࡃ 5)ࠊᮏ◊✲࡛ࡣᅇ㌿ᑐ⛠యࢆ௬ᐃࡋ࡚ゎᯒࡶ⾜ࡗࡓࠋJRR-3M, TNRF-2,୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ࢆ⏝࠸ࡓᵓ㐀ゎᯒ㻙㻌 㻟㻞㻟㻌㻙

ba

T

Cap bubble
Ellipsoidal bubble
Fig.1 Axial symmetrical bubble.

JAEA-Review 2011-050

Steam

Table 1 Experimental conditions

Reservoir
Run No.
Run 4
Run 5
Run 6
Run 7
Run 8
Run 9
Run 10
Run 11
Run 12
Run 13
Run 14

Tube Pump
Electric Heater

TC1

Steam Bubble
TC2
Test Section
TC3
View area

TC4

y

TC2
[qC]
105.8
109.0
111.7
115.3
118.7
124.3
125.2
129.6
134.7
140.2
144.0

TC3
[qC]
106.2
108.2
110.3
112.0
115.3
119.6
124.7
128.8
133.7
139.1
143.0

TC4
[qC]
106.1
107.2
107.5
108.5
110.0
112.2
121.7
121.8
129.5
136.2
138.2

TC5
[qC]
103.7
104.2
103.9
104.0
104.5
105.3
111.0
109.9
111.4
115.2
121.6

TC6
[qC]
100.1
100.2
100.0
100.0
100.0
100.6
102.0
102.4
101.8
101.4
104.1

Temperature Gradient('T/'y)ave [K/m]
25
40
64.5
80.5
107.5
142.5
137
188.5
223
239
213.5

Comments
Non boiling
Non boiling
Non boiling
Boiling
Boiling
Boiling
Boiling
Boiling
Boiling
Boiling
Boiling

Water Droplet

TC5

x

TC1
[qC]
104.4
107.4
111.2
115.3
120.2
125.0
125.0
130.2
134.8
140.5
144.1

Injection Nozzle

TC6
Aluminum Fin
Cooling Fan

Fig.2 Schematic of Experimental Apparatus.
3. ᐇ㦂⿦⨨ཬࡧᐇ㦂᪉ἲ
Fig.2 ࡟ᐇ㦂⿦⨨ࡢᴫ␎ࢆ♧ࡍࠋヨ㦂㒊ࡣ࢔࣑ࣝࢽ
࣒࢘〇▴ᙧᐜჾ㸦㧗ࡉ 600 mmࠊᖜ 100 mmࠊዟ⾜ࡁ
20 mm㸧࡛࠶ࡾࠊヨ㦂㒊ᗏ㒊࡟ࡣࢫࢸࣥࣞࢫ〇ᾮ⁲ᄇᑕࣀࢬࣝ㸦ෆᚄ 0.5 mm㸧ࡀタࡅࡽࢀ࡚࠸ࡿࠋ▴ᙧᐜჾୖ㒊࡟ࡣຍ⇕⏝㟁Ẽࣄ࣮ࢱࡀྲྀࡾ௜ࡅ࡚࠶ࡾࠊ
ヨ㦂㒊ୗ㒊ࡣ࢔࣑ࣝࢽ࣒࢘〇ࣇ࢕ࣥ࠾ࡼࡧ✵෭ࣇ࢓ࣥࡀྲྀࡾ௜ࡅࡽࢀ࡚࠶ࡿࠋᐜჾୖ㒊ࢆຍ⇕ࠊୗ㒊ࢆ෭༷ࡍࡿࡇ࡜࡟ࡼࡾࠊᆶ┤᪉ྥ࡟ ᗘ໙㓄ࢆⓎ⏕ࡉࡏࠊᏳᐃ࡞ᐦᗘᡂᒙࢆᐇ⌧ࡍࡿࡇ࡜ࡀ࡛ࡁࡿࠋὶయ

࡜ࡋ࡚ࡣࠊࢽ࣮ࣗࢺࣥྜ㔠㸦⼥Ⅼ 95Υ㸧࠾ࡼࡧ⣧Ỉࢆ⏝࠸ࡓࠋ ⁐⼥㔠ᒓࡢ ᗘィ ࡣࠊ࢔࣓ࣝࣝ㺃ࢡ࣓ࣟࣝ ⇕㟁ᑐ࡟ࡼ ࡾヨ㦂㒊ᗏ 㒊࠿ࡽ 2.5cm, 7.5cm,
10cm ࡢ 3 ಶᡤࡢ఩⨨࡛⾜ࡗࡓࠋᾮ⁲ὶ㔞ࡣࠊࢳ࣮ࣗ
ࣈ࣏ࣥࣉࡢᅇ㌿ᩘ࡟ࡼࡾㄪᩚࡋࡓࠋᐇ㦂ࡣᐜჾୗ㒊ࢆ⣙ 100Υ࡟ಖࡕࠊTable1 ࡟♧ࡍࡼ࠺࡟ᾮ⁲ὶ㔞࠾ࡼࡧᐜჾࡢୖ㒊 ᗘࢆኚ໬ࡉࡏ࡚⾜ࡗࡓࠋ
4. ᐇ㦂⤖ᯝཬࡧ⪃ᐹ
Fig.3 ࡟ᾮ⁲ࡢ⵨ⓎࡢᵝᏊࢆ♧ࡍࠋ᧜ീ㏿ᗘࡣẖ⛊
500 ࢥ࣐࡛࠶ࡿࡀࠊࡇࡇ࡛ࡣ 80ms ẖࡢ⏬ീࢆ࡞ࡽ࡭
࡚࠸ࡿࠋ⏬ീ୰ࡢ࡯࡜ࢇ࡝ࢆ༨ࡵࡿ⅊Ⰽࡢ㒊ศࡀ⁐⼥㔠ᒓࢆ♧ࡋࠊ▮༳ࡢඛ➃ࡢ㯮࠸Ⅼࡣᾮ⁲ࢆ♧ࡍࠋ
Run4 ࡣࠊୖୗࡢ ᗘᕪࡀᑠࡉࡃࠊᾮ⁲ࡣ⵨Ⓨࡍࡿࡇ࡜࡞ࡃ⁐⼥㔠ᒓ୰ࢆୖ᪼ࡍࡿࠋࡋ࠿ࡋࠊRun11ࠊRun13
࡟♧ࡍࡼ࠺࡟ୖୗࡢ ᗘᕪࡀ኱ࡁࡃ࡞ࡿ࡜┤᥋᥋ゐRun 4droplet

0ms

80ms

160ms

240ms

320ms

400ms

480ms

560ms

80ms

160ms

240ms

320ms

400ms

480ms

560ms

Run 11

0ms

Run 13
bubble

0ms

80ms

160ms

240ms

320ms

400ms

480ms

Fig.2 Water droplet evaporating in Newton's alloy taken by neutron radiography㻙㻌 㻟㻞㻠㻌㻙

560ms

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JAEA-Review 2011-050

5. ⤖ㄽ
୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ࢆ⏝࠸࡚ࡼࡾヲ⣽࡞ΰ┦ὶ◊✲ࢆ⾜࠺ࡓࡵ࡟ࠊ⁐⼥㔠ᒓ୰ࡢᾮ⁲ࡢ┤᥋᥋ゐ⵨Ⓨ⌧㇟ࢆᑐ㇟࡜ࡋ࡚ᐇ㦂ࢆ⾜࠸ࠊⓎ⏕ࡋࡓ஧┦ẼἻࡢᙧ≧ࡀᅇ㌿ᑐ⛠య࡜௬ᐃࡋ࡚ẼἻ⏬ീࡢᢳฟࢆ⾜ࡗࡓࠋ⤖ᯝ࠿ࡽࠊ༢࡞ࡿ஧್໬ฎ⌮࡛ࡣ⏺㠃ࡣࣀ࢖ࢬࡢᙳ㡪࡟ࡼࡾࢫ࣒࣮ࢬ࡛ࡣ࡞ࡃࠊ㜈್ࡢỴᐃࡶ㞴ࡋ࠸ࡀࠊᅇ㌿ᑐ⛠యࢆ௬ᐃࡋࡓゎᯒࡢሙྜ࡟ࡣࠊྛ
᫬้࡛ィ ࡋࡓయ✚ࢆ⏝࠸ࡿࡓࡵ࡟ゎᯒୖࠊྜ⌮ⓗ࡟⏺㠃఩⨨ࢆỴᐃࡍࡿࡇ࡜ࡀྍ⬟࡛࠶ࡗࡓࠋࡶࡕࢁ
ࢇࠊࡇࡢゎᯒ᪉ἲࡣᅇ㌿ᑐ⛠ࡀ௬ᐃ࡛ࡁࡿ᮲௳࡟ࡋ
࠿㐺⏝࡛ࡁ࡞࠸ࡇ࡜࡟ὀពࡍࡿᚲせࡀ࠶ࡿࠋFig.3 (a) Simple image binarization.

௒ᚋࡢ᪉㔪ࡇࢀࡲ࡛ᾮ⁲ࡢ┤᥋᥋ゐ⵨Ⓨ⌧㇟࡟ࡘ࠸࡚ࡣࠊ༢
୍ᾮ⁲ࢆ⏝࠸ࡓᐇ㦂ࢆ⾜ࡗ࡚ࡁࡓࡀࠊ௒ᚋࡣࡉࡽ࡟
⌧ᐇⓗ࡞ၥ㢟࡜ࡋ࡚ከᩘࡢᾮ⁲ࡀ⵨Ⓨࡍࡿሙྜࡢᐇ
㦂ࢆ⾜࠺ணᐃ࡛࠶ࡿࠋ⌧ᅾࠊᙜ◊✲ࢢ࣮ࣝࣉ࡛ࡣࠊ
ඹྠ฼⏝◊✲ࡢㄢ㢟࡜ࡋ࡚ࠕJRR-3M ⇕୰ᛶᏊࢆ฼
⏝ࡋࡓΰ┦ὶࡢືែィ ἲࡢ㧗ᗘ໬-IIࠖࢆ⾜ࡗ࡚࠸ࡿࡀࠊࡉࡽ࡟⥅⥆ࡋ࡚ࠊ௒ᚋࡶᛴ⃭࡞┦ኚ໬ࢆక࠺
ΰ┦ὶࡢィ ᢏ⾡ࡢ㛤Ⓨࢆ⾜࠸ࡓ࠸࡜⪃࠼࡚࠸ࡿࠋ

Fig.3 (b) Original image and calculated results.

Fig.3 (c) Calculated bubble shape.
Fig. 3. Consecutive bubble images.
⇕ఏ㐩࡟ࡼࡾᾮ⁲ෆ࡛⵨Ⓨࡀ㉳ࡇࡾࠊ஧┦ẼἻࡀ⏕ࡌ࡚࠸ࡿࡇ࡜ࡀࡼࡃࢃ࠿ࡿࠋࡉࡽ࡟⏬ീ࠿ࡽࠊ஧┦ẼἻࡣᴃ෇࠿ࡽ➟≧ẼἻ࡟ኚ໬ࡋ࡚࠸ࡿࡇ࡜ࡶ᫂░࡟ほᐹࡍࡿࡇ࡜ࡀ࡛ࡁࡿࠋᚑ᮶ࡢሗ࿌ 6)࡛ࡣྠࡌࡼ
࠺࡞య⣔࡛Ⓨ⏕ࡍࡿ஧┦ẼἻࡣ⦪㛗ࡢẼἻ࡜࡞ࡿࡇ
࡜ࡀሗ࿌ࡉࢀ࡚࠸ࡿࡀࡇࢀࡣࣀࢬࣝ㒊࡟࠾ࡅࡿ⵨Ẽᄇᑕ࡟ࡼࡿᙳ㡪࡟ࡼࡿࡶࡢ࡜⪃࠼ࡽࢀࡿࠋ
Fig.4 ࡣ⏬ീฎ⌮࡟ࡼࡿẼἻᙧ≧ࡢᢳฟ⤖ᯝࢆ♧
ࡍࠋFig.4(a)ࡣࠊ஧್໬࡟ࡼࡿ⏬ീฎ⌮࡛࠶ࡿࠋࡇࡢ
ฎ⌮࡛ࡣࠊẼἻࡢ⏺㠃ࡀࣀ࢖ࢬࡢᙳ㡪ࢆཷࡅ࡚⁥ࡽ࠿࡛ࡣ࡞ࡃࠊ஧್໬ࡢࡓࡵࡢ㜈್ࡶ⌮ㄽⓗ࡟Ỵᐃࡍࡿࡇ࡜ࡀ㞴ࡋ࠸ࠋFig.4(c)ࡣᅇ㌿ᑐ⛠ࢆ௬ᐃࡋࡓゎᯒ⤖ᯝࢆࠊFig.4(b)ࡣ⌧⏬ീ࡟ Fig.4(c)࡛ᚓࡽࢀࡓẼἻ
ࡢ㍯㒌ࢆ㔜ࡡ࡚⾲♧ࡋ࡚࠶ࡿࠋࡇࢀࡽࡢẼἻᙧ≧ࡢᢳฟ⤖ᯝ࠿ࡽࢃ࠿ࡿࡼ࠺࡟ᅇ㌿ᑐ⛠ࢆ௬ᐃࡋࡓィ⟬⤖ᯝࡣ⌧⏬ീࡢほᐹ⤖ᯝ࡜Ⰻࡃ୍⮴ࡍࡿࡇ࡜ࡀࢃ࠿
ࡿࠋࡲࡓࠊࡇࡢゎᯒ࡛ࡣ஧┦ẼἻࡢయ✚ࢆࡶ࡜࡟ẼἻᙧ≧ࢆ⟬ฟࡍࡿࡓࡵࠊྛ᫬้࡟࠾ࡅࡿయ✚ࡣᐇ㦂⤖ᯝ࡜ྠࡌ࡛࠶ࡿࠋᢳฟࡉࢀࡓẼἻࡢ㧗ࡉ࠾ࡼࡧᖜ
ࡶⰋࡃ୍⮴ࡋ࡚࠸ࡿࡇ࡜࠿ࡽࠊᮏᐇ㦂᮲௳࡛ࡣ஧┦ẼἻࢆᅇ㌿ᑐ⛠య࡜ࡋ࡚௬ᐃࡋ࡚ࡶⰋ࠸ࡇ࡜ࡀ♧၀
ࡉࢀࡓࠋ

ཧ⪃ᩥ⊩
[1] Y. Saito, K. Mishima, Y. Tobita, T. Suzuki, and M.
Matsubayashi, Proc. 9th Int. Symposium on Flow
Visualization, Edinburgh, U.K. 2000.
[2] W.B.Feller et al., "Gamma Insensitive Higly Borated
Microchannel Plates for Neutron Imaging”, Proc. 8thWorld
Conferenceon
NeutronRadiography,
Gaithersburg, Maryland, USA. Oct.16-19. 2006.
[3] K.-I. Mochiki et al., “Neutron Color Image
Intensifier”, , Proc. 8th World Conference on NeutronRadiography, Gaithersburg, Maryland, USA. Oct.16-19.
2006.
[4] Y. Saito et al., "Application of High Frame Rate
Neutron Radiography to Liquid-Metal Two-Phase Flow
Research," Nucl. Instrum. Methods Phys. Res. A,
vol.424, pp.229-234, 2005.
[5] Y. Saito et al., “Shape Measurement of Bubble in a
Liquid-Metal”, Proc. 6th Int. Topical Meeting on
Neutron Radiography, Kobe, Japan, Sept. 14-18,2008.
[6] Y.Nishi et al., Proc. 11th IHTC, Kyongju, Korea,
August 23-28, 1998
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JAEA-Review 2011-050

2-4ᶞᮌࡢ㜵ᚚ཯ᛂ࡜Ỉศືែ㻰㼑㼒㼑㼚㼟㼑㻌㻾㼑㼟㼜㼛㼚㼟㼑㼟㻌㼛㼒㻌㼀㼞㼑㼑㼟㻌㼍㼚㼐㻌㻰㼥㼚㼍㼙㼕㼏㼟㻌㼛㼒㻌㼃㼍㼠㼑㼞㻌㻰㼕㼟㼠㼞㼕㼎㼡㼠㼕㼛㼚㻌㻌ᮾி኱Ꮫ኱Ꮫ㝔㎰Ꮫ⏕࿨⛉Ꮫ◊✲⛉ ᒣ⏣฼༤ࠊỌ▼᠇㐨ࠊ⏣㔝஭៞ኴᮁࠊ୰す཭Ꮚ㻳㼞㼍㼐㼡㼍㼠㼑㻌㻿㼏㼔㼛㼛㼘㻌㼛㼒㻌㻭㼓㼞㼕㼏㼡㼘㼠㼡㼞㼍㼘㻌㼍㼚㼐㻌㻸㼕㼒㼑㻌㻿㼏㼕㼑㼚㼏㼑㼟㻘㻌㼠㼔㼑㻌㼁㼚㼕㼢㼑㼞㼟㼕㼠㼥㻌㼛㼒㻌㼀㼛㼗㼥㼛㻌㼀㻚㻌㼅㼍㼙㼍㼐㼍㻘㻌㻺㻚㻌㻺㼍㼓㼍㼕㼟㼔㼕㻘㻌㻷㻚㻌㼀㼍㼚㼛㼕㻌㼍㼚㼐㻌㼀㻚㻹㻚㻌㻺㼍㼗㼍㼚㼕㼟㼔㼕㻌I. ◊✲ࡢ┠ⓗ࡜ព⩏ ୰ᛶᏊ⥺ࡣỈ⣲୰࡛ࡢῶ⾶⋡ࡀ኱ࡁ࠸ࡇ࡜࠿ࡽࠊ
୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕㸦NRG㸧ἲࡣᶞᮌࡢᮦෆࢆࡣ
ࡌࡵ࡜ࡍࡿ᳜≀యෆࡢỈࡢศᕸࢆ㠀◚ቯⓗ࡟▱ࡿ᭷⏝࡞ᡭἲ࡛࠶ࡿࠋᶞᮌ࡛ࡣᮦࡢ⑓ኚ㒊࡛೺඲㒊࡜␗࡞ࡿỈศศᕸࢆ♧ࡍࡀࠊࡇࢀࡣᶞᮌࡢ㜵ᚚ཯ᛂ࡜ࡢ
㛵㐃ࡀ⪃࠼ࡽࢀࡿࡓࡵࠊ୧⪅ࡢ㛵ಀゎ᫂ࢆ┠ⓗ࡜ࡋࡓࠋ㠀◚ቯⓗ࡟Ỉศศᕸࡢኚ໬ࢆᤊ࠼ࡿࡇ࡜ࡀ࡛ࡁࢀ
ࡤࠊᶞᮌࡢデ᩿ࡸ⑓ែ⏕⌮➼ࡉࡲࡊࡲ࡞ᛂ⏝ࡀ⪃࠼ࡽࢀࡿࠋ౛࠼ࡤࠊ㔝እ࡟࠾ࡅࡿᶞᮌࡢಽቯࡢ༴㝤ᗘデ᩿࡟㡢㡪Ἴఏ㐩㏿ᗘࡸȚ⥺ࡢ㏱㐣⋡ ᐃࡀ⏝࠸ࡽࢀጞࡵ࡚࠸ࡿࠋࡇࢀࡽࢆྵࡵࠊ⭉ᮙ㒊ࠊ✵Ὕ㒊ࢆᤊ࠼ࡿࡓࡵࡢ㠀◚ቯデ᩿ἲࡣ⭉ᮙ⛬ᗘࡔࡅ࡛࡞ࡃỈศ➼ࡢᐦᗘศᕸ࡟ᕥྑࡉࢀࡿࠋᮦኚⰍ㒊ࠊ⭉ᮙ㒊ࡢỈศศᕸࡢࣃࢱ࣮ࣥࡣᶞ✀࡟ࡼࡗ࡚␗࡞ࡿࡇ࡜ࡀ᥎
ࡉࢀࠊデ᩿ࡢ☜ᗘࢆపࡃࡍࡿせᅉ࡜࡞ࡿࠋࡇࡢỈศศᕸࡢኚືࡢ᳨ฟࠊࡉࡽ࡟ࡑࡢཎᅉ࡜࡞ࡿᶞᮌࡢ⏕⌮ⓗ࡞཯ᛂࡢ㏣㊧ࢆᐇ㦂ⓗ࡟⾜࠺ࡓࡵ࡟ NRG ࡀ฼⏝࡛ࡁࡿ࡜⪃࠼ࡽࢀࡿࠋ
௒ᅇࡣࠊയᐖ࡟ᑐࡍࡿᶞᮌᮌ㒊ࡢ㜵ᚚ཯ᛂ࡜Ỉศศᕸࡀᶞ✀࡟ࡼࡗ࡚࡝ࡢࡼ࠺࡟␗࡞ࡿ࠿ࢆ▱ࡿࡓࡵ࡟ࠊ࠸ࡃࡘ࠿ࡢᶞ✀ࢆ⏝࠸ࠊࡲࡎ᭱ึ࡟⮬↛ࡢയᐖࢆཷࡅࡓᯞ࡛ࠊḟ࡟ඹ㏻ࡢேⅭⓗ࡞യᐖࢆ୚࠼ࡓ୺
ᖿ࠾ࡼࡧᯞ㸭ⱑᮌ࡛ࠊNRG ࡟ࡼࡿほᐹࢆ⾜ࡗࡓࠋ࡞࠾ࠊ௨ୗࡢᐇ㦂ࡣࡍ࡭࡚ JRR-3M 7R ࡢ TNRF ࢆ฼⏝ࡋ࡚⾜ࡗࡓࠋ⇕୰ᛶᏊࡢࣇࣛࢵࢡࢫࡣ 1.5×108
n/cm2/s ࡛࠶ࡿࠋII.⮬↛യᐖᯞࡢほᐹ1. ⥴ゝ
 ᶞᮌࡣ⮬↛࡟ࡶከࡃࡢᶵᲔⓗയᐖࢆཷࡅࡿࠋയᐖ
ࡢᙧ≧ࡣ୙ᐃ࡛࠶ࡿࡀࠊᶞ✀≉᭷ࡢ⤌⧊࡜཯ᛂ࡟ᇶ
࡙࠸ࡓയᐖ㒊ࡢᵝᘧࢆ♧ࡍࡣࡎ࡛࠶ࡿࠋࡑࡇ࡛ࠊࡲ
ࡎ⮬↛࡟യᐖࢆཷࡅࡓ✀ࠎࡢᶞᮌࡢᯞ࡟ࡘ࠸࡚㜵ᚚ㛵㐃⤌⧊ࡸỈศࡢศᕸࡀ࡝ࡢࡼ࠺࡟࡞ࡗ࡚࠸ࡿ࠿ࢆ
ㄪ࡭ࡓࠋ
2. ᐇ㦂
ᮾி኱Ꮫ㝃ᒓ₇⩦ᯘ⏣↓ヨ㦂ᆅ㸦すᮾிᕷ㸧࡛ࠊ

JRR-3M 7R ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕⿦⨨ࣉࣛࢱࢼࢫࠊࣄࣀ࢟ࠊ࢖ࣟࣁ࣑ࣔࢪࡢࠊ(㈈)᪂ᢏ⾡
㛤Ⓨ㈈ᅋ᳜≀◊✲ᅬ㸦⇕ᾏᕷ㸧࡛ࠊ࣐ࣖࣔࣔࠊࣖࣈ
ࢶࣂ࢟ࠊࢩࢲࣞࢨࢡࣛࡢയᐖᯞ㸦እ㒊࡟㟢ฟࡋࡓയࡢ࠶ࡿᯞ㸧ࢆ᥇ྲྀࡋࡓࠋ࢖࣓࣮ࢪࣥࢢࣉ࣮ࣞࢺ㸦IP㸧
࡛㏱㐣ീࢆࠊࡲࡓ CCD ࣓࢝ࣛ㸦200mm ࣞࣥࢬ㸧࡟
ࡼࡗ࡚ CT ീ㸦ᶓ᩿㠃࠾ࡼࡧ⦪᩿㠃㸧ࢆᚓࡓࠋྠࡌヨᩱ࡛᪂㩭᫬ࠊ஝⇱᫬ࢆẚ㍑ࡍࡿࡇ࡜ࡣ࡛ࡁ
࡞࠿ࡗࡓࡀࠊ࠸ࡎࢀࡢᶞ✀ࡶ᪂㩭࡞ヨᩱ࡜஝⇱ࡋࡓヨᩱࡢほᐹ࡛Ỉศࡸ㜵ᚚ㛵㐃≀㉁ࡢศᕸࢆ᳨ウࡋࡓࠋ
3. ⤖ᯝ
3-1. ㏱㐣ീࡢほᐹ ㏱㐣ീ㸦ᅗ-1㸧࡛ࡣ㔪ⴥᶞ㸦ࣄࣀ࢟㸧࡜ᗈⴥᶞࡢ
≉ᚩࢆ༊ูࡍࡿࡇ࡜ࡣ࡛ࡁ࡞࠿ࡗࡓࠋᯞඛᯤࢀࡢሙ
ྜࡣᗈⴥᶞ࡛ࡶ஝⇱ࡀ㐍ࡴࡓࡵ NRG ࡛⏕Ꮡ㒊࡜༊ูࡍࡿࡇ࡜ࡀ࡛ࡁࡓࠋࡲࡓࠊ㜵ᚚ㛵㐃≀㉁ࡢ㞟✚࡟ࡘ࠸࡚ࡣയᐖࡢ᪉ྥ࡟ࡼࡗ࡚ࡣ༑ศ☜ㄆ࡛ࡁࡓࠋ

᪂㩭ᯞ㸦⏣↓ヨ㦂ᆅ㸧   ஝⇱ᯞ㸦⏣↓ヨ㦂ᆅ㸧ୖ࠿ࡽࣉࣛࢱࢼࢫࠊࣄࣀ࢟ࠊ࣑ࣔࢪ㸦ྛ 2 ᮏ㸧᪂㩭ᯞ㸦᳜≀◊✲ᅬ㸧   ஝⇱ᯞ㸦᳜≀◊✲ᅬ㸧ୖ࠿ࡽ࣐ࣖࣔࣔࠊࣖࣈࢶࣂ࢟ࠊࢩࢲࣞࢨࢡࣛ㸦ྛ 2 ᮏ㸧ᅗ-1. ⮬↛യᐖᯞࡢ㏱㐣ീᶞᮌ་Ꮫ㻙㻌 㻟㻞㻢㻌㻙

ࢫࢱࣥࢲ࣮ࢻࡣࢸࣇࣟࣥࡢࢫࢸࢵࣉ

JAEA-Review 2011-050

 ᯞࡀ୙ᩚᙧࡢ෇ᰕ≧࡛࠶ࡿࡇ࡜࡟ຍ࠼ࠊࡉࡽ࡟ᙧ
ែࡢኚ␗࡟ᐩࡴയᐖ㒊ࢆ༢࡞ࡿ㏱㐣ീ࡛ゎᯒࡍࡿࡢࡣᅔ㞴࡛࠶ࡗࡓࠋࡇ࠺ࡋࡓᯞࡢゎᯒ࡟ࡣ CT ീࡢᵓ⠏ࡀᚲせ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡿࠋ
3-2. CT ീࡢほᐹയᐖ㒊ࡢ୰ᚰ௜㏆࡛᭱ࡶയᐖࡀ㢧ⴭ࡞㒊఩ࡢᶓ᩿㠃ࢆ CT ീ࡟ࡼࡾほᐹࡋࡓ㸦ᅗ-2㸧ࠋࡲࡓࠊ⦪᩿㠃࡛ࡢほᐹࡶ⾜ࡗࡓ㸦ᅗ-3㸧ࠋ஝⇱ヨᩱࡢほᐹ࠿ࡽࠊ࡝ࡢᶞ✀ࡶ⑓ኚ㒊㸦ᮦኚⰍ㒊㸧ࡢ࿘ᅖ࡟୙᥹Ⓨᛶࡢ≀㉁ࡀ㞟✚㸦㜵ᚚ㛵㐃≀㉁࡜⪃࠼ࡽࢀࡿ㸧ࡋ࡚࠸ࡿࡇ࡜ࡀศ࠿ࡗࡓࠋ≉࡟㔪ⴥᶞࡢࣄࣀ࡛࢟㢧ⴭ࡛࠶ࡗࡓࠋࡇࡢ≀㉁ࡢ㞟✚ࡣ᪂㩭ヨᩱ࡛ࡣỈศ࡟ࡼࡗ࡚࣐ࢫࢡࡉࢀ୙᫂░࡟࡞ࡗࡓࡇ
࡜࠿ࡽࠊỈศࠊ㜵ᚚ㛵㐃≀㉁ࡢ୧⪅ࡢศᕸ≧ἣࢆ▱ࡿ࡟ࡣ᪂㩭ヨᩱ࡜஝⇱ヨᩱ࡜ࢆẚ㍑ࡍࡿᚲせࡀ࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋ
㔪ⴥᶞࡢࣄࣀ࡛࢟ࡣ㜵ᚚ⤌⧊ࢆྵࡴ⑓ኚ㒊࡛ྵỈ⋡ࡢపୗࡀ☜ㄆࡉࢀࡓࠋࡋ࠿ࡋࠊᗈⴥᶞࡢࣉࣛࢱࢼ
ࢫࠊ࣑ࣔࢪࠊࣖࣈࢶࣂ࢟ࠊ࣐࡛ࣖࣔࣔࡣྵỈ⋡ࡢపୗࡣ୙᫂░࡛࠶ࡗࡓࠋࡲࡓࠊࢩࢲࣞࢨࢡ࡛ࣛࡣ㏫࡟㜵ᚚ㛵㐃≀㉁࡜࡜ࡶ࡟Ỉࡢ㞟✚ࡢྍ⬟ᛶࡀࡳࡽࢀࡓࠋ
4. ࡲ࡜ࡵ
ྠࡌヨᩱࡢ᪂㩭᫬࡜஝⇱᫬ࡢẚ㍑ࡣ࡛ࡁ࡞࠿ࡗࡓ
ࡀࠊ࠾࠾ࡲ࠿࡞ྛᶞ✀ࡢയᐖᵝᘧࡢ≉ᚩࢆࡘ࠿ࡴࡇ
࡜ࡀ࡛ࡁࡓࠋയᐖ㒊ෆ㒊ࡢᵝᏊࢆ㠀◚ቯ࡛ほᐹࡍࡿࡇ࡜࡛ࠊയᐖࡢᒚṔࡲ࡛࠶ࡿ⛬ᗘ᥎ ྍ⬟࡛࠶ࡗࡓࠋ
⑓ኚ㒊࡜Ỉศ࡜ࡢ㛵ಀ࡟ࡘ࠸࡚ࡣᗈⴥᶞ㛫࡛ࡣ኱ࡁ࡞ᕪ␗ࡀ࡞࠿ࡗࡓࡀࠊ㔪ⴥᶞ࡜ᗈⴥᶞ࡜࡛኱ࡁࡃ␗
࡞ࡗ࡚࠸ࡓࠋ

ࣉࣛࢱࢼࢫ

ࣄࣀ࢟࢖ࣟࣁ࣑ࣔࢪ       ࢩࢲࣞࢨࢡࣛ

ࣖࣈࢶࣂ࢟       ࣐ࣖࣔࣔᅗ-2. ⮬↛യᐖᯞࡢᶓ᩿㠃 CT ീ ࡑࢀࡒࢀࠊᕥࡀ᪂㩭ヨᩱࠊྑࡀ஝⇱ヨᩱࣉࣛࢱࢼࢫ       ࣄࣀ࢟࢖ࣟࣁ࣑ࣔࢪ㸦ᯞඛᯤ㸧  ࢩࢲࣞࢨࢡࣛ

ࣖࣈࢶࣂ࢟      ࣐ࣖࣔࣔᅗ-3. ⮬↛യᐖᯞࡢ⦪᩿㠃 CT ീ ࡑࢀࡒࢀࠊᕥࡀ᪂㩭ヨᩱࠊྑࡀ஝⇱ヨᩱIII.ேⅭയᐖᮌࡢほᐹ
1. ⥴ゝയᐖ࡟ᑐࡍࡿᶞᮌࡢ཯ᛂ࡜Ỉศศᕸࡢኚ໬ࠊᮦ⤌⧊ᵓ㐀࡜ࡢ㛵㐃ࢆゎ᫂ࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡋ࡚ࠊྛ✀ᶞᮌ࡟ேⅭⓗ࡞യᐖࢆ୚࠼ࡿヨ㦂ࢆ⾜ࡗࡓࠋ2. ᐇ㦂
⿇ࣨᾆᕷ࡟࠶ࡿ㸦ᰴ㸧ᐩኈ᳜ᮌ㛗ᾆᅡሙ࡛ࠊኟᏘ
࡟㔪ⴥᶞࡢ࢖ࢳࣙ࢘㸦ࡇࡇ࡛ࡣ㔪ⴥᶞ࡜ࡋ࡚ᢅ࠺㸧ࠊ࢝ࣖࠊᗈⴥᶞࡢ࣐ࢸࣂࢩ࢖ࠊࢩࣛ࢝ࢩ㸦௨ୖࠊᨺᑕ
Ꮝᮦ㸧ࠊࢧࣝࢫ࣋ࣜࠊࣄ࣓ࢩࣕࣛࠊࢧࢡࣛ㸦㛵ᒣ㸧ࠊࢱࣈࣀ࢟㸦௨ୖࠊᩓᏍᮦ㸧ࡢィ 8 ✀ࡢᶞᮌࡢ୺ᖿ࡟
ᚄ 15mm ࡢࢻ࡛ࣜࣝࠊࡲࡓᯞ࠶ࡿ࠸ࡣⱑᮌ࡟ᚄ
2.5mm ࡢࢻ࡛ࣜࣝ㈏㏻ࡍࡿ✸Ꮝയᐖࢆຍ࠼ࡓࠋയᐖ
ࡢ 1 㐌㛫ࠊ2 ࠿᭶ࠊ1 ᖺࠊ3 ᖺᚋ࡟യᐖ㒊ࢆ᥇ྲྀࡋࡓࠋ
୺ᖿࡣ⣙ 10㹼12mm ཌࡢ෇ᯈ࡟ࡋ࡚ IP ࢆ⏝࠸࡚㏱㐣
ീࢆほᐹࡋࡓࠋᯞ࠶ࡿ࠸ࡣⱑᮌࡣ㛗ࡉ⣙ 20cm ࡟ษ
᩿ࡋ࡚ࠊCCD ࣓࢝ࣛ㸦105mm ࣞࣥࢬ㸧࡛᧜ീࡋ CTീࢆᵓ⠏ࡋࡓࠋ
Ỉศࡸ㜵ᚚ㛵㐃≀㉁ࡢศᕸࣃࢱ࣮ࣥࢆ᫂ࡽ࠿࡟ࡍ
ࡿࡓࡵࠊୖグヨᩱࡢ࠸ࡎࢀࡶ᪂㩭ヨᩱ࡜⤯஝ヨᩱࡢ
ほᐹࢆ⾜ࡗࡓࠋ
3. ⤖ᯝ
3-1. ୺ᖿ㒊ࡢയᐖ㸫ᶞᮌ෇ᯈࡢ㏱㐣ീ 2-4

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JAEA-Review 2011-050

 ୺ᖿ㒊ࡢയᐖ 1 㐌㛫ᚋࡢほᐹ౛ࢆᅗ-4 ࡟ࠊ3 ᖺᚋࡢほᐹ౛ࢆᅗ-5 ࡟♧ࡍࠋ 㔪ⴥᶞࡢ࢖ࢳࣙ࢘ࡸ࡛࢝ࣖࡣ 1 㐌㛫ᚋࡢᮦኚⰍࡣ
᫂░࡛࡞ࡃࠊᗈࡀࡗ࡚ࡶ࠸࡞࠿ࡗࡓࠋᮦኚⰍࡣ 2 ࠿᭶ᚋ࡟ࡣ᫂░࡟࡞ࡾࠊࡑࡢ㛗ࡉࡣ 2 ࠿᭶௨㝆ࡶᣑ኱ࡋࡓࠋ࢖ࢳ࡛ࣙ࢘ࡣ 1 㐌㛫ᚋ࠿ࡽᮦኚⰍ㒊ࡢ஝⇱ࡀㄆࡵࡽࢀࡓࠋ࡛࢝ࣖࡣ஝⇱㒊ࡣ 2 ࠿᭶ᚋࠊ1 ᖺᚋ࡛
ࡶ㏱㐣ീ࡛☜ㄆࡉࢀ࡞࠿ࡗࡓࡀࠊ3 ᖺᚋࡢヨᩱ࡛ࡣㄆࡵࡽࢀࡓࠋ
ᗈⴥᶞ࡟ࡘ࠸࡚ࡳࡿ࡜ࠊࣄ࣓ࢩ࡛ࣕࣛࡣࠊ1 㐌㛫ᚋ࡟ࡣᮦኚⰍ㒊ࡀ᫂░࡟ㄆࡵࡽࢀࠊ2 ࠿᭶ᚋ࡟ࡣࡉ
ࡽ࡟⃰ࡃ࡞ࡗࡓࠋࡋ࠿ࡋࠊᮦኚⰍࡢ኱ࡁࡉࡣ㍈᪉ྥࠊ᥋⥺᪉ྥ࡜ࡶ࡯࡜ࢇ࡝ᗈࡀࡿࡇ࡜ࡣ࡞࠿ࡗࡓࠋ㏱㐣
ീ࡛ࡣᮦኚⰍ㛵㐃ࡢ஝⇱㒊ࡣ඲ࡃㄆࡵࡽࢀ࡞࠿ࡗࡓ
ࡀࠊയࡢ࿘ᅖࡢ≀㉁㸦Ỉ࠶ࡿ࠸ࡣ㜵ᚚ㛵㐃≀㉁㸧ࡢ㞟✚ࡣ 1 㐌㛫ᚋ࡟ࡣ᪤࡟ࡳࡽࢀࡓࠋ࣐ࢸࣂࢩ࢖ࡸࢩ
ࣛ࢝ࢩࡶᮦኚⰍ㒊ࡢᙧᡂ࣭ᣑ኱࠶ࡿ࠸ࡣയࡢ࿘ᅖࡢ≀㉁ࡢ㞟✚࡟ࡘ࠸࡚ࡣࣄ࣓ࢩࣕࣛ࡜ྠᵝ࡛࠶ࡗࡓࠋ
ࡓࡔࡋࠊ࣐ࢸࣂࢩ࢖࡛ࡣ 1 㐌㛫ᚋࡢᮦኚⰍࡣࡸࡸⷧ
ࡃࠊࡑࡢ㍈᪉ྥࡢ㛗ࡉࡣ 2 ࠿᭶ࢆ㉺࠼࡚ࡶᣑ኱ࡋࡓࠋ
ࢱࣈࣀ࢟ࡶୖグᗈⴥᶞ࡜ྠᵝ࡛࠶ࡗࡓࡀࠊ1 㐌㛫ᚋࡢᮦኚⰍࡣࡸࡸⷧ࠿ࡗࡓࠋ1 㐌㛫ᚋࡢᖿ࡛ࡣ⫗║࡛㍈᪉ྥ࡟஝⇱㒊ࡀࡳࡽࢀࡓࡀࠊ㏱㐣ീ࡛ࡣ☜ㄆ࡛ࡁ࡞࠿ࡗࡓࠋᮦኚⰍࡢ㍈᪉ྥࡢ㛗ࡉࡣ 2 ࠿᭶ࢆ㉺࠼࡚ࡶᣑ኱ࡋࡓࠋയࡢ࿘ᅖࡢ≀㉁ࡣ㏱㐣ീ࡛᫂░࡛࠶ࡾࠊ≉࡟ 1 ᖺᚋ࡛ୖୗ࡟ఙ㛗ࡋ࡚࠸ࡓࠋࢧࢡࣛࡶᮦኚⰍ
ࡣ 1 㐌㛫ᚋ࡛᫂░࡛ࠊᮦኚⰍࡢࡑࡢ௚ࡢ≉ᚩࡸ≀㉁ࡢ㞟✚࡟ࡘ࠸࡚ࡣ௚ࡢᗈⴥᶞ࡜ྠᵝ࡛࠶ࡗࡓࠋ1 㐌㛫ᚋ࡟⫗║࡛ෆᒙ࠿ࡽࡢ஝⇱ࡀࡳࡽࢀࡓࡀ㏱㐣ീ࡛ࡣ୙᫂░࡛࠶ࡗࡓࠋࢧࣝࢫ࣋ࣜࡶᮦኚⰍࡣ 1 㐌㛫࡛᫂░࡛ࠊᮦኚⰍࡢࡑࡢ௚ࡢ≉ᚩࡸ≀㉁ࡢ㞟✚࡟ࡘ࠸࡚ࡣ௚ࡢᗈⴥᶞ࡜ྠᵝ࡛࠶ࡗࡓࠋ

ᮦኚⰍ୙᫂░

஝⇱ヨᩱ  ᮦኚⰍ᫂░  ஝⇱ヨᩱ࢖ࢳࣙ࢘         ࢩࣛ࢝ࢩᅗ-4. യᐖ 1 㐌㛫ᚋࡢᮦኚⰍ࡜஝⇱ヨᩱࡢ NRG ീയᐖ 3 ᖺᚋࡢほᐹ࡛ࡶࠊࡍ࡭࡚ࡢᶞ✀ࡢ஝⇱ヨᩱ
࡛യᐖ 2 ࠿᭶ᚋࠊ1 ᖺᚋ࡜ྠࡌࡃᮦኚⰍ㒊ࡢ࿘ᅖ࡟ᙧᡂࡉࢀࡓ཯ᛂ㞀ቨ࡟㜵ᚚ㛵㐃≀㉁࡜᥎ ࡉࢀࡿ୙᥹Ⓨᛶ≀㉁ࡢ㞟✚ࡀㄆࡵࡽࢀࡓࠋ
࡛࢝ࣖࡣയᐖ 1 ᖺᚋ࡜␗࡞ࡾࠊ࢖ࢳࣙ࢘࡜ྠᵝ࡞㔪ⴥᶞ࡟୍⯡ⓗ࡞ኚ໬ࠊࡘࡲࡾയᐖ㒊࿘ᅖࡢᮦኚⰍ

㒊ࡢ஝⇱ࡀほᐹࡉࢀࡓࠋࡲࡓࠊࢱࣈࣀ࡛࢟ࡣ 1 ᖺᚋ࡟ࢃࡎ࠿࡟ㄆࡵࡽࢀࡓᮦኚⰍ㒊࡬ࡢỈࡢ㞟✚ࡀ㢧ⴭ࡟࡞ࡗࡓࠋ௚ࡢᗈⴥᶞࠊࢩࣛ࢝ࢩࠊࢧࢡࣛࠊࢧࣝࢫ
࡛࣋ࣜࡣ௜യ 1 ᖺᚋ࡜ྠࡌࡃᮦኚⰍ㒊ࡢ஝⇱ࡶỈࡢ㞟✚ࡶㄆࡵࡽࢀ࡞࠿ࡗࡓࠋ

࢝ࣖࡢᮦኚⰍ  ஝⇱ヨᩱ   ᪂㩭ヨᩱࢧࢡࣛࡢᮦኚⰍ  ஝⇱ヨᩱ   ᪂㩭ヨᩱࢱࣈࣀ࢟ࡢᮦኚⰍ ஝⇱ヨᩱ   ᪂㩭ヨᩱ

ᅗ-5. യᐖ 3 ᖺᚋࡢᮦኚⰍ࡜ NRG ㏱㐣ീ ḟ࡟ࠊ㔪ⴥᶞ࡜ᗈⴥᶞࡢ௦⾲౛࡜ࡋ࡚࢖ࢳࣙ࢘࡜
ࢱࣈࣀ࢟ࡢയᐖ 1 ᖺᚋࡢヨᩱ࡟ࡘ࠸࡚୰ᛶᏊ㏱㐣ᗘࢆࢢࣛࣇ໬ࡋࡓ㸦ᅗ-6㸧ࠋ ࢖ࢳ࡛ࣙ࢘ࡣࢱࣈࣀ࢟࡟ẚ࡭ඖࠎࡢྵỈ⋡ࡀ㧗࠸ࡀࠊᮦኚⰍ㒊࡛ࡣᴟ➃࡟஝⇱㸦ࢢࣛࣇࡢ୰ኸࡢ❑ࡳ࡛ࡣ᪂㩭ヨᩱ࡜஝⇱ヨᩱࡢ⥺ࡀ㏆᥋㸧ࡋࡓࡢ࡟ᑐࡋࠊ
ࢱࣈࣀ࡛࢟ࡣᮦኚⰍ㒊ࡢ஝⇱ࡣㄆࡵࡽࢀ࡞࠿ࡗࡓࠋ
ࢱࣈࣀ࡛࢟ࡣയᐖᏍࡀ࠶ࡿ࡟ࡶ࠿࠿ࢃࡽࡎ࣐ࢫࢡࡉ
ࢀࡿ࡯࡝࡞ࢇࡽ࠿ࡢ≀㉁ࡢ㞟✚ࡀ㢧ⴭ࡛࠶ࡾࠊᮦኚ
Ⰽ㒊࡛Ỉศࡀቑຍࡋ࡚࠸ࡿࡼ࠺࡛࠶ࡿࠋ ஝⇱ヨᩱ࡛㜵ᚚ㛵㐃≀㉁࡟ࡘ࠸࡚ࡳࡿ࡜ࠊ࢖ࢳࣙ
࡛࢘ࡣᮦኚⰍ㒊ࡢ࿘ᅖ࡟ⷧ࠸ᖏ≧࡟㞟✚ࡀࡳࡽࢀࠊ
ࡑࡇࡼࡾෆഃࡀ஝⇱ࡋ࡚࠸ࡓࠋࢱࣈࣀ࡛࢟ࡣ࢖ࢳࣙ
࢘࡯࡝㢧ⴭ࡛࡞࠸ࡀ㞟✚ࡀㄆࡵࡽࢀࡓࠋ
௨ୖࡢࡼ࠺࡟ࠊᮦኚⰍࡣയᐖ 1 㐌㛫ᚋ࡛ࡣ≉࡟㔪ⴥᶞ࡛ࡣ୙᫂░࡛࠶ࡗࡓࡀࠊ2 ࠿᭶ᚋ௨㝆ࡣ࡝ࡢᶞ✀ࡶ᫂░࡟࡞ࡗࡓࠋỈᖹ᪉ྥࡢᮦኚⰍࡢ⠊ᅖࡣ࡝ࡢᶞ✀ࡶ࡯࡜ࢇ࡝ᗈࡀࡽ࡞࠿ࡗࡓࠋ࢖ࢳ࡛ࣙ࢘ࡣയᐖ
㒊ࡢ࿘ᅖ࡛᪩ࡃ࠿ࡽ஝⇱㒊ࡀㄆࡵࡽࢀࡓࡀࠊྠࡌ㔪ⴥᶞ࡛ࡶ࡛࢝ࣖࡣ஝⇱㒊ࡢᙧᡂࡣᬑ㐢ⓗ࡛࡞࠸࠿㐜࠿ࡗࡓࠋᗈⴥᶞ࡛ࡣᮦኚⰍࡀ⏕ࡌ࡚ࡶയᐖ㒊࿘ᅖࡢ஝⇱ࡣ࡯࡜ࢇ࡝ㄆࡵࡽࢀࡎࠊࢱࣈࣀ࢟ࡢࡼ࠺࡟㏫࡟Ỉࡢ㞟✚ࡀ᥎ ࡉࢀࡿᶞ✀ࡀ࠶ࡗࡓࠋ㔪ⴥᶞࠊᗈⴥ

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JAEA-Review 2011-050

ᶞ࡜ࡶᮦኚⰍ㒊ࡢቃ⏺࡛㜵ᚚ㛵㐃≀㉁࡜ᛮࢃࢀࡿ୙
᥹Ⓨᛶ≀㉁ࡢ㞟✚ࡀ 1 㐌㛫ᚋ࡟ࡣࡍ࡭࡚ࡢᶞ✀࡛ㄆࡵࡽࢀࠊࡑࡢ㔞ࡣ᫬㛫ࡢ⤒㐣࡜࡜ࡶ࡟ቑຍࡋࡓࠋ㜵ᚚ⤌⧊ᙧᡂࡢ᫬㛫⤒㐣ࡀྠࡌ࡛࠶ࡗ࡚ࡶᮦኚⰍ㒊ࡢỈศศᕸࡀᶞ✀࡟ࡼࡗ࡚␗࡞ࡿࡇ࡜ࡀ☜ㄆࡉࢀࡓࠋ

ࡗࡓࠋCT ࡛ࡶ⑓ኚ㒊ࡢ࿘ᅖ࡟࠾ࡅࡿ㜵ᚚ㛵㐃≀㉁ࡢ㞟✚ࡣ࡝ࡢᶞ✀ࡶയᐖ 1 㐌㛫ᚋ࡟ࢃࡎ࠿࡟ࡳࡽࢀࠊ2࠿᭶ᚋ࡟ࡣቑຍࡋ࡚㢧ⴭ࡟࡞ࡗࡓࠋ
യᐖ 1 㐌㛫ᚋ࢖ࢳࣙ࢘    ᪂㩭ヨᩱ   ஝⇱ヨᩱയᐖ㸰࠿᭶ᚋ

࢖ࢳࣙ࢘

യᐖ 1 ᖺᚋ

ࢱࣈࣀ࢟    ᪂㩭ヨᩱ   ஝⇱ヨᩱ

࢖ࢳࣙ࢘

ࢱࣈࣀ࢟

࢝ࣖ

ࢩࣛ࢝ࢩ ࣐ࢸࣂࢩ࢖ ࢱࣈࣀ࢟ ࢧࢡࣛ

ᅗ-7. യᐖᯞ᪂㩭ヨᩱࡢ⦪᩿㠃 CT ീ

ᅗ-6. യᐖ 1 ᖺᚋࡢയᐖ㒊㸦ⓑ⥺㒊㸧ࡢ୰ᛶᏊ㏱㐣㜼ᐖᗘ㟷⥺㸸᪂㩭ヨᩱࠊ㉥⥺㸸஝⇱ヨᩱ

3-2. ⱑᮌ㸭ᯞࡢയᐖ㒊ࡢ CT ほᐹ᪂㩭ヨᩱࡢ⦪᩿㠃᩿ᒙീࡢ౛ࢆᅗ-7 ࡟♧ࡍࠋ㔪ⴥᶞ㸸࢖ࢳ࡛ࣙ࢘ࡣയᐖ 1 㐌㛫ᚋ࡟ࡣ CT ࡛᪤࡟㍈᪉ྥ࡟㛗࠸᫂░࡞஝⇱㒊ࡀほᐹࡉࢀࠊࡑࡢᚋࡢ
ᣑ኱ࡣㄆࡵࡽࢀ࡞࠿ࡗࡓࠋ୍⯡࡟ᮦኚⰍ㸦≉࡟യᐖࡢࡳ࡟㉳ᅉࡍࡿᮦኚⰍ㸧ࡣ᥋⥺᪉ྥࡢᣑ኱ࡣᑠࡉࡃ
᥋⥺᪉ྥ࡟㛗࠸ࡀࠊ⦪᩿㠃ࡢ CT ീほᐹࡀ᭷ຠ࡛࠶
ࡿࡇ࡜ࡀ☜ㄆࡉࢀࡓࠋ࡛࢝ࣖࡣ CT ࡛ࡶ஝⇱㒊ࡣࡳࡽࢀࡎࠊᗈⴥᶞ࡜ྠࡌࡼ࠺࡞ീ࡛࠶ࡗࡓࠋ ᗈⴥᶞ㸸ࡍ࡭࡚ࡢᗈⴥᶞ࡛യᐖ㒊ࡢ࿘ᅖ࡟஝⇱㒊ࡣㄆࡵࡽࢀ࡞࠿ࡗࡓࠋയࡢ࿘ᅖࡢ≀㉁㸦Ỉ࠶ࡿ࠸ࡣ㜵ᚚ㛵㐃≀㉁㸧ࡢ㞟✚ࡶ CT ࡛☜ㄆࡉࢀࡓࠋ≉࡟ࢱࣈࣀ࢟ࡢ 1 ᖺᚋ࡛ୖୗ࡟ఙ㛗ࡋ࡚࠸ࡿࡢࡀ㢧ⴭ࡛࠶ḟ࡟ࠊയᐖ 1 ᖺᚋࡢ᪂㩭ヨᩱ࡜஝⇱ヨᩱ࡜ࡢẚ㍑
㸦Ỉ࡜㜵ᚚ㛵㐃≀㉁ࡢศᕸࣃࢱ࣮ࣥ㸧ࢆᅗ-8 ࡟♧ࡍࠋ㔪ⴥᶞ࡛ࡣࠊ࢖ࢳ࡛ࣙ࢘௜യ㒊ࡢ࿘ᅖ࡟᪩ࡃ࠿ࡽ
ᮦኚⰍ㒊ࡼࡾᗈ࠸⦪㛗ࡢ஝⇱㒊ࡀᙧᡂࡉࢀࡓࠋࡇࢀ
ࡣࠊࢫࢠࠊࣄࣀ࡛࢟ࡳࡽࢀࡿ஝⇱㒊࡜ඹ㏻࡜⪃࠼ࡽࢀࡿࠋࡋ࠿ࡋࠊ㔪ⴥᶞ࡛ࡶ࡛࢝ࣖࡣࡇࡢࡼ࠺࡞஝⇱㒊ࡣࡳࡽࢀ࡞࠿ࡗࡓࠋࢩࣛ࢝ࢩ㸦ᨺᑕᏍᮦࠊᖖ⥳ᶞ㸧ࠊࢧࢡࣛ㸦ᩓᏍᮦࠊⴠⴥᶞ㸧ࠊࣄ࣓ࢩࣕࣛ㸦ᩓᏍᮦࠊⴠⴥᶞ㸧࡜࠸ࡗࡓᗈⴥᶞ࡛ࡣᮦኚⰍࡀ⏕ࡌ࡚ࡶയᐖ
㒊࿘ᅖࡢ஝⇱ࡣ࡯࡜ࢇ࡝ㄆࡵࡽࢀ࡞࠿ࡗࡓࠋࢱࣈࣀ
࢟㸦ᩓᏍᮦࠊᖖ⥳ᶞ㸧࡛ࡣ㏫࡟Ỉࡢ㞟✚ࡀ᥎ ࡉࢀࡓࠋ⤯஝≧ែ࡟ࡋࡓヨᩱࡢほᐹ࡛ࡣࠊIP ࡟ࡼࡿほᐹ⤖ᯝ࡜ྠࡌࡃࠊ㔪ⴥᶞࠊᗈⴥᶞ࡜ࡶᮦኚⰍ㒊ࡢቃ⏺࡛㜵ᚚ㛵㐃≀㉁࡜ᛮࢃࢀࡿ≀㉁ࡢ㞟✚ࡀ 1 㐌㛫ᚋ࡟ࡣࡍ࡭࡚ࡢᶞ✀࡛ㄆࡵࡽࢀࠊࡑࡢ㔞ࡣ᫬㛫ࡢ⤒㐣࡜࡜㻙㻌 㻟㻞㻥㻌㻙

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JAEA-Review 2011-050

ࡶ࡟ቑຍࡋࡓࠋ
ᩓᏍᮦ㸦୍㒊༙⎔Ꮝᮦ㸧࡜ᨺᑕᏍᮦ࡜࡛ඹ㏻ࡍࡿ
≉ᚩࡣ࡞࠿ࡗࡓࠋỈศศᕸ࡟ᕪ␗ࢆ⏕ࡌࡿᶵᵓࡸࠊ
ᕪ␗࡜ᶞᮌࡢᵓ㐀ࡸ⏕⌮ⓗᛶ㉁࡜ࡢ㛵㐃ࢆ᳨ウࡍࡿ
ᚲせࡀ࠶ࡿࠋᮏሗ࿌࡛ࡣ┬␎ࡍࡿࡀࠊ୍ࡘࡢヨࡳ࡜ࡋ࡚ྛᶞ✀ࡢയᐖ㒊ࡢ⤌⧊໬Ꮫⓗほᐹࢆ⾜ࡗ࡚࠸ࡿࠋ

࢖ࢳࣙ࢘     ࢝ࣖ㔪ⴥᶞ      㔪ⴥᶞࢩࣛ࢝ࢩ     ࢱࣈࣀ࢟     ࢧࢡࣛᨺᑕᏍᮦ    ᩓᏍᮦ    ᩓᏍᮦᅗ-8. യᐖ 1 ᖺᚋࡢ⦪᩿㠃 CT ീ ࡑࢀࡒࢀࠊᕥࡀ஝⇱ヨᩱࠊྑࡀ᪂㩭ヨᩱ

4. ࡲ࡜ࡵ
ᮦኚⰍࡣയᐖᚋḟ➨࡟᫂░࡟࡞ࡗࡓࠋᮦኚⰍࡢ኱
ࡁࡉࡣࠊỈᖹ᪉ྥ࡛ࡣ࡝ࡢᶞ✀ࡶ࡯࡜ࢇ࡝ᗈࡀࡽ࡞
࠿ࡗࡓࡀࠊ㍈᪉ྥ࡟㛗ࡃ࡞ࡗࡓࠋ࢖ࢳ࡛ࣙ࢘ࡣയᐖ
㒊ࡢ࿘ᅖ࡛᪩ࡃ࠿ࡽ㍈᪉ྥ࡟㛗࠸஝⇱㒊ࡀㄆࡵࡽࢀ
ࡓࠋࡇࢀࡣࡇࢀࡲ࡛ࡢࢫࢠࡸࣄࣀ࡛࢟ࡢ◊✲⤖ᯝ࡜୍⮴ࡋከࡃࡢ㔪ⴥᶞ࡟ඹ㏻ࡍࡿ≉ᚩ࡜⪃࠼ࡽࢀࡓࡀࠊ
࡛࢝ࣖࡣ᫂░࡛࡞࠿ࡗࡓࠋ௚ࡢ㔪ⴥᶞ࡟ࡘ࠸࡚ࡶ࡝
ࡕࡽࡢࢱ࢖ࣉ࠿☜ㄆࢆせࡍࡿࠋᗈⴥᶞ࡛ࡣᮦኚⰍࡀ
⏕ࡌ࡚ࡶയᐖ㒊࿘ᅖࡢ஝⇱ࡣ࡯࡜ࢇ࡝㉳ࡇࡽࡎࠊ㏫࡟Ỉࡢ㞟✚ࡀ᥎ ࡉࢀࡿᶞ✀ࡀ࠶ࡗࡓࠋ㔪ⴥᶞࠊᗈⴥᶞ࡜ࡶᮦኚⰍ㒊ࡢቃ⏺࡛㜵ᚚ㛵㐃≀㉁࡜ᛮࢃࢀࡿ
ᅛᙧ≀ࡢ㞟✚ࡀ 1 㐌㛫ᚋ࡟ࡣࡍ࡭࡚ࡢᶞ✀࡛ㄆࡵࡽࢀࠊࡑࡢ㔞ࡣ᫬㛫ࡢ⤒㐣࡜࡜ࡶ࡟ቑຍࡋࡓࠋ

ࢀࡓࠋ௒ᚋࡣࠊNRG ௨እࡢᡭἲ࡛ࡶࡗ࡚ࠊᮌ㒊ࡢ⤌⧊ᵓ㐀࠶ࡿ࠸ࡣ㜵ᚚ཯ᛂࡢࢱ࢖ࣉ࡜Ỉศศᕸ࡜ࡢ㛵㐃ࢆ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࡀᚲせ࡛࠶ࡿࠋࡲࡓࠊᶞ✀࡟ࡼࡿỈศศᕸࡢᕪ␗ࡀ☜ㄆࡉࢀࡓࡇ
࡜࠿ࡽࠊ⌧ሙ࡛ࡢ㠀◚ቯᡭἲ࡟ࡼࡿ⭉ᮙデ᩿࡛ࡣࡇࡢⅬࢆ⪃៖ࡍࡿᚲせࡀ࠶ࡿࠋᏘ⠇࠶ࡿ࠸ࡣỈࢫࢺࣞࢫ࡟ࡼࡗ࡚ࡶỈศศᕸࡀኚࢃࡿࡇ࡜ࡀண᝿ࡉࢀࡿࡢ
࡛ࠊࡇࡢኚ໬ࢆ NRG ࡟ࡼࡗ᳨࡚ฟࡍࡿࡇ࡜ࡶ௒ᚋ
ࡢㄢ㢟࡛࠶ࡿࠋ
V. ᡂᯝࡢබ⾲
Yamada, T., Yamato, M. & Nakanishi, T.M. (2005)
Influence of water stress on lesion expansion in thexylem of Cryptomeria japonica seedlings inoculatedwith a canker fungus Guignardia cryptomeriae
revealed by neutron radiography. International Forest
Review 7(5):373 (XXII International Union of Forest
Research Organizations World Congress Abstract)ᒣ⏣฼༤ (2005) ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕࡛ぢࡿᶞᮌᮌ㒊ࡢയᐖ࡟ᑐࡍࡿ཯ᛂ. ➨ 3 ᅇ᪥㡑୰ᛶᏊࣛࢪ
࢜ࢢࣛࣇ࢕࣮࣡ࢡࢩࣙࢵࣉࠕ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ
࢕ࠖᑓ㛛◊✲఍㸦ᖹᡂ 17 ᖺᗘ㸧ሗ࿌᭩:128-143
Yamada, T. (2006) Influence of water stress and wetnessof open wound on lesion expansion in the xylem of
Cryptomeria japonica seedlings inoculated with acankerfungusGuignardia
cryptomeriae.8th
International Mycological Congress Abstracts
Book:179ᒣ⏣฼༤࣭Ọ▼᠇㐨࣭ᒣୗᚓ⏨࣭ᑠᒣᖖኵ࣭⚄ᗞṇ๎࣭኱ᓥ Ώ (2006) ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕࡛ࡳ
ࡓയᐖᚋࡢᶞᮌࡢỈศ࡜㜵ᚚ⤌⧊ࡢኚ໬. ➨ 11 ᅇᶞᮌ་Ꮫ఍኱఍ㅮ₇せ᪨㞟 11:69
ᒣ⏣฼༤ (2007) ᶞᮌࡢ୰ࢆデࡿ㸫ᮦኚⰍ⭉ᮙ㜵Ṇ࡜ṇ☜࡞༴㝤ᗘデ᩿ࡢࡓࡵ࡟㸫. ࢢ࣮࢚࣮ࣜࣥࢪ
2007 ᖺ 1 ᭶ྕ:30-33ᒣ⏣฼༤࣭Ọ▼᠇㐨࣭ᒣୗᚓ⏨࣭ᑠᒣᖖኵ࣭⚄ᗞṇ๎࣭኱ᓥ Ώ࣭㣤಴ ᐶ (2007) ྛ✀ᶞᮌ࡟࠾ࡅ
ࡿയᐖᚋࡢỈศศᕸࡢኚ໬࠾ࡼࡧ㜵ᚚ⤌⧊ᙧᡂ.
➨ 118 ᅇ᪥ᮏ᳃ᯘᏛ఍኱఍Ꮫ⾡ㅮ₇㞟:46

IV. ௒ᚋࡢㄢ㢟 ᪂㩭ヨᩱ࡜஝⇱ヨᩱ࡜ࡢẚ㍑ࠊ≉࡟ CT ࡟ࡼࡗ࡚⑓ኚ㒊ࡢ᩿ᒙീࢆᚓࡿࡇ࡜࡛ࠊᶞ✀࡟ࡼࡿ⑓ኚ㒊࠶ࡿ࠸ࡣ㜵ᚚ཯ᛂⓎ⌧㒊఩ࡢ≉ᛶࡢ㐪࠸ࡀ᫂░࡟♧ࡉ㻙㻌 㻟㻟㻜㻌㻙

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2-5୰ᛶᏊ࢖࣓࣮ࢪ࣭࢖ࣥࢸࣥࢩࣇ࢓࢖࢔ࡢࡓࡵࡢື⏬᧜ീࢩࢫࢸ࣒ࡢ㛤Ⓨ
Development of Imaging System for Neutron Image Intensifierᣢᮌᖾ୍ࠊ࿴⏣Ὀ᫂ࠊᒸᓮ㐨ᙪ
K. Mochiki, Y. Wada and M. OkazakiṊⶶᕤᴗ኱Ꮫ Musashi Institute of Technology㸬ࡣࡌࡵ࡟
ᖹᡂ 16 ᖺᗘ࠿ࡽ 17 ᖺᗘ࡟࠿ࡅ࡚ 2 ᖺ㛫࡛⾜ࡗࡓ୰ᛶᏊ࢖࣓࣮ࢪ࣭࢖ࣥࢸࣥࢩࣇ࢓࢖࢔㸦㹇㹇㸧ࡢᛶ⬟ヨ㦂ࡣᴟࡵ࡚Ⰻዲ࡞⤖ᯝࡀᚓࡽࢀࡓࠋࡇࡢ
ᡂᯝࢆࡩࡲ࠼ࠊ㹒㹌㹐㹄㸰࡟࠾ࡅࡿື⏬᧜ീ⏝ࡢ᧜ീ⣔ࡢᩚഛࢆ⾜࠸ࠊ㧗㏿㹁㹒ࠊࡦ࠸࡚ࡣࢲ࢖ࢼ
࣑ࢵࢡ㹁㹒⏝ࡢ㧗ᛶ⬟࡞᧜ീࢩࢫࢸ࣒ࡢ㛤Ⓨࢆ⾜ࡗࡓࡢ࡛ሗ࿌ࡍࡿࠋ
㸬୰ᛶᏊ㹇㹇ࢆ⏝࠸ࡓ୰ᛶᏊ㹁㹒ᚑ᮶ࡢ୰ᛶᏊ⏝⺯ගࢥࣥࣂ࣮ࢱ࡜㧗ឤᗘ࣓࢝ࣛ
࠿ࡽᡂࡿ᧜ീ⿦⨨࡛ࡣࠊ୰ᛶᏊࡢ᳨ฟຠ⋡ࡀᝏ࠸ࡓࡵ࡟⤫ィⓗ࡞ᦂࡽࡂࡀከࡃࠊࡺ࠼࡟㹁㹒⏝ࡢࢹ࣮ࢱࢆᚓࡿ࡟ࡣ㛗᫬㛫࠿ࡅ࡚᧜ീࡍࡿࡢࡀ୍⯡ⓗ࡛࠶ࡿࠋ㸱ḟඖ㹁㹒࡛ࡣ෌ᵓᡂฎ⌮ࡢࡓࡵ࡟ከᩘ
ࡢ㏱㐣ീࢆᚲせ࡜ࡍࡿࡓࡵࠊ᧜ീసᴗࡣ㛗᫬㛫࡟ཬࡧࠊࡲࡓ⿕᳨యࡢᨺᑕ໬ࡶၥ㢟࡜࡞ࡗ࡚࠸ࡿࠋ
୰ᛶᏊ࢖࣓࣮ࢪ࣭࢖ࣥࢸࣥࢩࣇ࢓࢖࢔㸦௨ୗ୰ᛶᏊ㹇㸬㹇㸬㸧ࡣࡇࢀࡽࡢḞⅬࢆඞ᭹ࡍࡿ᧜ീ⿦⨨࡛࠶ࡿࠋ୰ᛶᏊ࡟ᑐࡋ㧗࠸᳨ฟຠ⋡ࢆᣢࡕࠊࡼࡾ
▷᫬㛫࡛᧜ീసᴗࢆ⾜࠼ࡿࡼ࠺࡟࡞ࡿ[1,2]ࠋ
୰ᛶᏊ㹁㹒ࢩࢫࢸ࣒
୰ᛶᏊ㹇㸬㹇㸬ࢆ⏝࠸ࡓ㹁㹒⏝୰ᛶᏊ㏱㐣ീ᧜ᙳࢩࢫࢸ࣒ࡢᵓᡂࢆᅗ㸯࡟♧ࡍ[3]ࠋ⿕᳨యࢆ㏱㐣
ࡋ࡚ࡁࡓ୰ᛶᏊࡣ᧜ീ⿦⨨࡟ࡼࡗ࡚ྍど໬ࡉࢀࠊࡑࡢീࢆ᧜ീ⣲Ꮚ㸦࣓࢝ࣛ➼㸧࡟ࡼࡗ࡚᧜ᙳࡍࡿࠋ
㹁㹒ࡢ෌ᵓᡂฎ⌮ࢆ⾜࠺ࡓࡵ࡟ࡣࠊ⿕᳨యࢆᵝࠎ

ࡾࠊ30fps ࡛ 8bit ࡶࡋࡃࡣ 10bit ࢢ࣮ࣞࢫࢣ࣮ࣝ
⏬ീࢆ᧜ᙳ࡛ࡁࡿࠋ㹁㹁㹂࣓࢝ࣛࡢ⏬⣲ᩘࡣ
640x480 ⏬⣲࡛࠶ࡾࠊ㹂㹔㹂ࣅࢹ࢜ࢹࢵ࢟࡟ 30fps
࡛ 8bit ࢢ࣮ࣞࢫࢣ࣮ࣝື⏬࡜ࡋ࡚グ㘓ࡋࡓࠋࡲࡓ
ẚ㍑⏝࡜ࡋ࡚ࠊ୰ᛶᏊ㹇㸬㹇㸬࡛ࡣ࡞ࡃ⺯ගᯈ࡟ࡼࡿᚑ᮶ࡢ᧜ീ⿦⨨ࢆ⏝࠸࡚㛗᫬㛫᧜ീࡶ⾜ࡗ࡚
㏱㐣ീࢆྲྀᚓࡋࡓࠋࡇࡢ᧜ᙳ࡟ࡣ὾ᯇ〇 C4880 ෭༷ᆺ㹁㹁㹂࣓࢝ࣛࢆ⏝࠸ࡓࠋࡑࡢ⏬⣲ᩘࡣ
1024x1024 ⏬⣲㸦1008x1023 ࡛ฎ⌮㸧࡛࠶ࡾࠊ32bitࢢ࣮ࣞࢫࢣ࣮ࣝ⏬ീࢆ᧜ᙳ࡛ࡁࡿࠋࡼࡗ࡚௒ᅇࡢ
ᐇ㦂࡛ࡣࠊ㹁㹒⏝㏱㐣ീࢆ㸱✀㢮ࡢ᮲௳࡛ࡑࢀࡒ
ࢀྲྀᚓࡋࡓࠋࡑࡢ᧜ീ᮲௳ࢆ⾲㸯࡟♧ࡍࠋ⾲㸯 ᧜ീ᮲௳
᧜ീ⣲Ꮚ㻌෭༷ᆺ䠟䠟䠠
䠏ᯈᘧ䜹䝷䞊
䠟䠟䠠㻌
䠟䠩䠫䠯㻌

᧜ീ⿦

⏬ീ㻌

᧜ീ㻌

᧜ീ

⨨㻌

ゎീᗘ㻌

᫬㛫㻌

ᯛᩘ

㻝㻜㻜㻤㼤㻝㻜㻞㻟㻌 㻣㻞㻜㻜 ⛊

㻢㻜㻜

⺯ගᯈ㻌
୰ᛶᏊ䠥䠥

㻢㻠㻜㼤㻠㻤㻜㻌

㻝㻤 ⛊

㻡㻠㻜

୰ᛶᏊ䠥䠥

㻝㻞㻤㻜㼤㻝㻜㻞㻠㻌

㻥⛊

㻞㻣㻜


⿕᳨య࡜ࡋ࡚ࠊ⊂⮬࡟〇సࡋࡓ෇⟄ᙧࡢ㹁㹒ゎീᗘホ౯⏝࢖ࣥࢪࢣ࣮ࢱࢆ౑⏝ࡋࡓࠋ࢖ࣥࢪࢣ࣮ࢱ
ࡣ࢔࣑ࣝࢽ࣒࢘〇࡛࠶ࡾࠊෆ㒊࡟ࡣᵝࠎ࡞ᙧ≧࣭኱ࡁࡉࡢ✵ὝࡀᏑᅾࡋࠊࡑࡢ୍㒊࡟ࡣ㕲࡞࡝ࡀᇙࡵ㎸ࡲࢀ࡚࠸ࡿࠋᐇ㦂ࢆ⾜ࡗࡓ᪋タࡣ᪥ᮏཎᏊຊ
◊✲㛤Ⓨᶵᵓ㸦㹈㸿㹃㸿㸧ࡢ㹈㹐㹐㸫㸱㹋࡛࠶ࡿࠋࡇࡇ࡛ࡣ㹊㸭㹂㸻㸯㸵㸴࡛࠶ࡾࠊ↷ᑕࡉࢀࡿ⇕୰82ᛶᏊ᮰ࡣ 1.5 u 10 n / cm  s ࡛࠶ࡿࠋ
୰ᛶᏊ࢖࣓࣮ࢪ࢖ࣥࢸࣥࢩࣇ࢓࢖࢔࡞ゅᗘ࠿ࡽ᧜ᙳࡋࡓ㏱㐣ീࡀ༙ᅇ㌿ศࡔࡅᚲせ࡜࡞ࡿࠋࡼࡗ࡚ᅗ࡟♧ࡍࡼ࠺࡟⿕᳨యࡣࢱ࣮ࣥࢸ࣮
୰ᛶᏊ㹁㹒࡛ࡣࠊ୰ᛶᏊ࡛ᚓࡽࢀࡿ㏱㐣ീࡢ⏬
ࣈࣝୖ࡟⨨࠿ࢀࠊࢸ࣮ࣈࣝࢆ୍ᐃ㏿ᗘ࡛ᅇ㌿ࡉࡏ㉁ࡀࠊ㹖⥺࡜␗࡞ࡾ㔞Ꮚⓗᦂࡽࡂᡂศࡢࣀ࢖ࢬࡢ
࡞ࡀࡽ⿕᳨య࡟୰ᛶᏊ⥺ࢆ↷ᑕࡋࠊ㐃⥆࡛㏱㐣ീᙳ㡪ࡀᙉࡃཷࡅࡿࡓࡵࠊ᧜ീ⣔࡟ࡣ㧗࠸᳨ฟຠ⋡ࢆ᧜ᙳࡋࡓࠋ
ࡀồࡵࡽࢀࡿࠋᚑ᮶ࡢ᧜ീ⿦⨨࡛ࡣࠊGd 2 O2 S ; Tb
 ᐇ㦂࡛ࡣ㏱㐣ീࡢ᧜ᙳ࡟ EPIX ♫〇 SV9M001
6
ࡸ LiF; ZnS ࡢ୰ᛶᏊ⏝⺯ගᯈࢆ⏝࠸ࡿࡢࡀ୍⯡ࡢ㹁㹋㹍㹑ࣅࢹ࣓࢜࢝ࣛ࡜ࠊ≉ู࡟ㄪᩚࡉࢀࡓᮾ
ⓗ࡛࠶ࡿࠋࡇࡢ᪉ᘧࡢᵓᡂࢆᅗ㸰࡟♧ࡍࠋࡇࡢ᪉
Ⱚ〇㸱ᯈᘧ࣮࢝ࣛ㹁㹁㹂ࣅࢹ࣓࢜࢝ࣛࢆ౑⏝ࡋࡓࠋᘧ࡛ࡣࠊ⺯ගࢆࣞࣥࢬ࡛㞟ගࡍࡿ㐣⛬࡛ග㔞ࡀ኱㹁㹋㹍㹑࣓࢝ࣛࡢ⏬⣲ᩘࡣ 12801024 ⏬⣲࡛࠶ᖜ࡟ῶᑡࡍࡿࡢ࡛ࠊ᳨ฟ㔞Ꮚຠ⋡ࡀపୗࡋ࡚ࡋࡲ
㹈㹐㹐㸫㸱㹋 㸵㹐 ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ ⿦⨨ ࠊ୰ᛶᏊ㹁㹒ࠊ࢖࣓࣮ࢪࣥࢢ㻙㻌 㻟㻟㻝㻌㻙

JAEA-Review 2011-050

㹁㹁㹂࣓࢝ࣛ࡟ࡼࡗ࡚᧜ീࡉࢀࡓ㏱㐣ീࡣࠊ㸱ᯛ࠺࡜࠸࠺ḞⅬࡀ࠶ࡿࠋᖹᆒ཰㞟⺯ගගᏊᩘࢆȜࠊࡈ࡜ࡢ୰ᚰ್ࢆ࡜ࡗ࡚㹁㹒⏝ࡢ㸯㸶㸮ᯛࡢ㏱㐣ീ୰ᛶᏊ᮰ࢆȭ࡜ࡍࢀࡤࠊࡇࡢ᪉ᘧ࡛ࡢ୰ᛶᏊࡢ᳨
ฟຠ⋡ࡣ S / N v I / 1  1 / H ࡜࡞ࡿࠋࡼࡗ࡚ࠊ ࡜ࡋ࡚࠸ࡿࠋ㹁㹋㹍㹑࡟ࡼࡗ࡚ᚓࡽࢀࡓ㏱㐣ീ࡟ࡣ❆ᖜ 3x3 ࡢ࣓ࢹ࢕࢔ࣥࣇ࢕ࣝࢱࢆ࠿ࡅ࡚࠸ࡿࠋ
ࡇࡢ᪉ᘧ࡛ࡣ༑ศ࡞ග㔞ࢆᚓࡿࡓࡵ࡟㛗᫬㛫࠿ࡅࡑࡢᚋࠊྛ㏱㐣ീ࡟ࡘ࠸࡚ᬯ㟁ὶ⿵ṇ࣭ࢩ࢙࣮ࢹ
࡚᧜ീࢆ⾜࠺ࡢࡀ୍⯡ⓗ࡛࠶ࡿࠋ࢕ࣥࢢ⿵ṇࢆ⾜࠺ࠋᬯ㟁ὶ⿵ṇ࣭ࢩ࢙࣮ࢹ࢕ࣥࢢ
⿵ṇ๓ࡲ࡛ࡢྛ᧜ീἲࡈ࡜ࡢ㏱㐣ീࢆᅗ㸳࡟♧ࡍࠋࡇࢀ࡟ᑐࡋ࡚ࠊ୰ᛶᏊ࢖࣓࣮ࢪ࣭࢖ࣥࢸࣥࢩࣇShepp-Logan ࣇ࢕ࣝࢱ⿵ṇࢆ⾜ࡗࡓᚋ࡟㔜␚࢓࢖࢔ࡣ୰ᛶᏊ⥺ࡢ᳨ฟ㔞Ꮚຠ⋡ࡀ㧗࠸᧜ീ⣔࡛✚ศἲ࡟ࡼࡾ෌ᵓᡂࢆ⾜ࡗࡓࠋ෌ᵓᡂ⏬ീ࡟ࠊ࢔࠶ࡿࠋᅗ㸱ࠊᅗ 4 ࡟ࡑࢀࡒࢀ୰ᛶᏊ㹇㸬㹇㸬ࡢእ࣑ࣝࡢ㒊ศࡀ㍤ᗘ㸯㸮㸮࡟ࠊ㕲ࡢ㒊ศࡀ㍤ᗘ㸰㸮ほ࡜ᵓ㐀ࢆ♧ࡍࠋࡇࢀࡣࠊᖹᡂ 15 ᖺᗘ࡟ᰴᘧ఍
㸮࡟࡞ࡿࡼ࠺࡟⿵ṇࡋࡓࡶࡢࢆᅗ㸴࡟♧ࡍࠋ♫ᮾⰪࡀヨసࡋࡓࡶࡢࢆ㉎ධࡋࡓࡶࡢ࡛࠶ࡿࠋ୰
෌ᵓᡂࢆ⾜ࡗࡓ┤ᚄ 60mm ࡢ࢔࣑ࣝᯈࡢ㒊ศᛶᏊ㹇㸬㹇㸬ࡣࠊධᑕࡋ࡚ࡁࡓ୰ᛶᏊࢆྍどග࡟࡟ࡣ┤ᚄ 2.0mmࠊ1.5mmࠊ1.0mm ࡢ✰ࡀࡑࢀࡒኚ᥮ࡍࡿࡔࡅ࡛࡞ࡃࠊᚤᙅ࡞ගࢆ᫂ࡿࡃࡍࡿᶵ⬟ࢀ㸯㸮ಶࡎࡘ㛤࠸࡚࠾ࡾࠊࡑࡢ࠺ࡕ㸳ࡘࡎࡘ࡟㕲ࢆᣢࡗࡓ኱ᆺࡢ㟁Ꮚ⟶(┿✵⟶)࡛࠶ࡿࠋ୰ᛶᏊ⥺ࡀᇙࡵ㎸ࡲࢀ࡚࠸ࡿࠋࡲࡓ࢔࣑ࣝᯈࡢ࿘ᅖ࡟ࡣ⣬※࠿ࡽᨺฟࡉࢀࡓ୰ᛶᏊࡣ⿕᳨యࢆ㏱㐣ࡋ࡚୰ᛶࡀᕳ࠿ࢀ࡚࠸ࡿࠋᏊ  㹇㸬㹇㸬࡟ධᑕࡍࡿࠋධຊ⺯ග㠃ࡣࠊ୰ᛶ෭༷ᆺ㹁㹁㹂࠾ࡼࡧ㹁㹋㹍㹑ࡢ෌ᵓᡂ⏬ീ࡛ࡣᏊ࡟ᑐࡋ࡚㧗ឤᗘ࡞⺯ගయࡀ᥇⏝ࡉࢀ࡚࠾ࡾࠊධ
㕲࡜✵Ὕࡢ୧᪉ࡢ㒊ศࡀ☜ㄆ࡛ࡁࡿࠋࡋ࠿ࡋ㸱ᯈᑕࡋࡓ୰ᛶᏊࡣ୰ᛶᏊᙉᗘ(୰ᛶᏊࡢಶᩘ)࡟ᛂࡌ
ᘧ㹁㹁㹂ࡢ෌ᵓᡂ⏬ീ࡛ࡣ✵Ὕ㒊ศࡣ☜ㄆ࡛ࡁ࡞ࡓග࡟ኚ᥮ࡉࢀࠊ⺯ග㠃⾲㠃ࡢග㟁⭷࡛ග㟁Ꮚࢆ࠿ࡗࡓࠋࡲࡓࠊྛ෌ᵓᡂ⏬ീ࠿ࡽ࢔࣑ࣝ㒊ศࡢ୍ᨺฟࡍࡿࠋග㟁Ꮚࡣ཰᮰㟁ᴟཬࡧ㝧ᴟ࡛ᵓᡂࡉࢀ
㒊ࢆᢤࡁฟࡋࠊࡑࡢᶆ‽೫ᕪࢆồࡵࡓࠋࡑࡢ⤖ᯝࠊࡿ㟁Ꮚࣞࣥࢬࡢస⏝࡛ࠊຍ㏿ࡉࢀ࡚ฟຊ⺯ග㠃࡟㸱ᯈᘧ㹁㹁㹂ࡢ෌ᵓᡂ⏬ീ࡛ࡣ෭༷ᆺ㹁㹁㹂ࡢ㸯.
㞟᮰ࡉࢀࡿࠋຍ㏿ࡉࢀࡓ㟁Ꮚࡣฟຊ⺯ග㠃ࢆບ㉳㸲㸰ಸࠊ㹁㹋㹍㹑ࡣ෭༷ᆺ㹁㹁㹂ࡢ㸯.㸮㸴ಸ࡜࡞ࡋ࡚ྍどീ࡟ኚ᥮ࡉࢀࡿࠋࡑࡢ㝿࡟㍤ᗘቑಸࡀ㉳ࡗࡓࠋࡇࢀ࡟ࡼࡾࠊ୰ᛶᏊ㹇㸬㹇㸬ࢆ⏝࠸࡚㹁㹋ࡇࡾࠊ㉥Ⰽᡂศࡢᙉ࠸㧗㍤ᗘࡢྍどീ࡜࡞ࡿࠋᚑ
㹍㹑࣓࡛࢝ࣛྲྀᚓࡉࢀࡓ㏱㐣ീࡣࠊᚑ᮶ࡢ᧜ീ᪉
᮶ࡢ᧜ീ᪉ᘧ࡜㐪࠸ࠊ᧜ᙳࡉࢀࡿྍどീ࡟ࡣගࡢ
ἲ࡛ྲྀᚓࡋࡓ㏱㐣ീ࡜ẚ࡭࡚ࡶࡉ࡯࡝ရ㉁ࡢຎࡽ
ศᩓࡢᙳ㡪ࡀᑡ࡞ࡃࠊᖹᆒ཰㞟⺯ගගᏊᩘȜࡀ༑࡞࠸ࢹ࣮ࢱ࡛࠶ࡿ࡜࠸࠼ࡿࠋ
ศ኱ࡁࡃ࡞ࡾ↓どࡉࢀࡿࡓࡵࠊ୰ᛶᏊࡢ᳨ฟຠ⋡ࡣ S / N v I ࡜࡞ࡿࠋ୰ᛶᏊ I.I.࠿ࡽࡢฟຊ⏬ീࡣࠊ୺࡟㉥Ⰽᡂศ࡛ᵓᡂࡉࢀ࡚࠸ࡿࡀࠊⱝᖸ⥳Ⰽࠊ
3. ࡲ࡜ࡵ
㟷ⰍࡢἼ㛗ᡂศࡶྵࡲࢀ࡚࠸ࡿࠋࡇࡢ࣮࢝ࣛ⏬ീࢆ㹐㹅㹀ᡂศࡑࢀࡒࢀࢆูࠎ࡟᧜ᙳࡍࢀࡤࠊⓎග ᐇ㦂࡟ࡼࡾࠊ୰ᛶᏊ㹇㹇ࢆ⏝࠸ࢀࡤഹ࠿㸷⛊ࡢᙉᗘࡢ㐪࠸࠿ࡽࠊࡑࢀࡒࢀឤᗘࡢ␗࡞ࡿ㉥(R)ࠊ⥳᧜ീ᫬㛫࡛ྲྀᚓࡋࡓ㏱㐣ീࢹ࣮ࢱ࡛ࡶࠊ㛗᫬㛫᧜(G)ࠊ㟷(B)ࡢ⏬ീࢆྠ᫬࡟ྲྀᚓ࡛ࡁࡿࠋࡓࡔࡋࠊ
ീ࡟ࡼࡾྲྀᚓࡉࢀࡿࢹ࣮ࢱ࡜ࡉ࡯࡝ရ㉁ࡢຎࡽ࡞
௒ᅇฎ⌮࡛౑⏝ࡋࡓ㏱㐣ീࡣ㉥⏬ീࡢࡳ࡜ࡋࡓࠋ
࠸㹁㹒෌ᵓᡂ⏬ീࡀᚓࡽࢀࡿࡇ࡜ࡀᐇドࡉࢀࡓࠋ ୰ᛶᏊ㹇㸬㹇㸬ࡢど㔝ࡣ㸷ࠊ㸴ࠊཬࡧ㸲.㸳࢖ࣥࢳᚄ࡛ྍኚ࡛࠶ࡿࠋど㔝ࢆ㸷࢖ࣥࢳࡢ≧ែ࡟ࡍࡿ
࡜ᶓ 18.29 cmࠊ⦪ 13.72cm ࡢど㔝࡛ࡢ᧜ീࡀྍ⬟ཧ⪃ᩥ⊩࡜࡞ࡗ࡚࠸ࡿࠋධᑕ㠃ࡢ⺯ගయࡣ Gd 2 O2 S ; Tb ࡛࠶ࡾࠊฟຊ⺯ග㠃࡟ࡣ Eu ࢆῧຍࡋࡓ㧗㍤ᗘ㉥ⰍⓎ1) ᣢᮌࠊᯇᮏࠊ⳥ụࠊᶫ㸹ᖹᡂ 17 ᖺᗘࠕ୰ᛶᏊ
ගయࡢ Y2 O2 S ; Eu ࢩࣥࢳ࣮ࣞࢱࡀ౑⏝ࡉࢀ࡚࠸ࡿࠋ
ࣛࢪ࢜ࢢࣛࣇ࢕ࠖᑓ㛛◊✲఍ࠊி኱ཎᏊ⅔ᐇ㦂ᡤ㉥ⰍⓎගࣆ࣮ࢡࡣᅛయ᧜ീ⣲Ꮚࡢឤᗘ≉ᛶ࡟㐺ྜ
(2005)
ࡋ࡚࠾ࡾࠊᚑ᮶ࡢ⥳Ⰽ⺯ගయࢆ౑⏝ࡋࡓ㹇㸬㹇㸬2) ᣢᮌᖾ୍ࠊᯇᮏဴ⏨ࠊ⳥ụ⚽ࠊᶫᗣ㐩ࠊ୰⚄㈼
࡜ẚ㍑ࡋࠊᩘಸࡢឤᗘᨵၿࡀ࡞ࡉࢀ࡚࠸ࡿࠋኈ ࠕ୰ᛶᏊ࢖࣓࣮ࢪ࢖ࣥࢸࣥࢩࣇ࢓࢖࢔ࢆ⏝࠸ࡓ୰ᛶᏊ㹁㹒ࠖ ᪥ᮏ㠀◚ቯ᳨ᰝ༠఍ ᖹᡂ 18 ᐃ⤖ᯝᖺᗘ᫓Ꮨ኱఍ pp.135-136 (2006)
3) ᣢᮌᖾ୍ࠊ᪥ሪග୍ ࠕ୰ᛶᏊ࣮࢝ࣛ࢖࣓࣮ࢪ
෭༷ᆺ㹁㹁㹂࣓࢝ࣛ࡟ࡼࡗ࡚᧜ീࡉࢀࡓ㏱㐣ീ࢖ࣥࢸࣥࢩࣇ࢓࢖࢔ࠖ ᛂ⏝≀⌮ࠊvol.75ࠊ㸴㸮㸮ᯛ࠿ࡽࠊ㸱ᯛࡈ࡜ࡢ᭱ᑠ್ࢆ࡜ࡗ࡚㸯ᯛࡢ
No.11 pp.1349-1353 (2006)
2-5⏬ീࢆసᡂࡋࠊ㸰㸮㸮ᯛࡢ㏱㐣ീ࡜ࡋ࡚ࡑࡢ࠺ࡕ
㸯㸶㸮ᯛࢆ㹁㹒෌ᵓᡂ࡟౑⏝ࡍࡿࠋ㸱ᯈᘧ࣮࢝ࣛ㻙㻌 㻟㻟㻞㻌㻙

JAEA-Review 2011-050

୰ᛶᏊᅛయ᧜ീ⣲Ꮚ䠄䠟䠟䠠, 䠟䠩䠫䠯䜲䝯䞊䝆䝉䞁䝃䠅

⿕᳨య䝍䞊䞁䝔䞊䝤䝹᧜ീ⿦⨨⏬ീ䝕䞊䝍䠄୰ᛶᏊ䜲䝯䞊䝆
䜲䞁䝔䞁䝅䝣䜯䜲䜰䠅ᅗ㸯 㹁㹒⏝୰ᛶᏊ㏱㐣ീ᧜ᙳࢩࢫࢸ࣒ࡢᵓᡂᅗ

ྍどග

ධᑕ୰ᛶᏊ

㙾

䠟䠟䠠䜹䝯䝷⺯ගᯈᅗ㸰 ᚑ᮶ࡢ᧜ᙳ⿦⨨ᅗ㸱 ୰ᛶᏊ㹇㸬㹇㸬ࡢእほ㻙㻌 㻟㻟㻟㻌㻙

2-5

JAEA-Review 2011-050

ධຊ❆
ฟຊ⺯ග㠃

ධᑕ୰ᛶᏊ

ග㟁
Ꮚ

ධຊ㠃

ฟຊග

ධᑕ୰ᛶᏊ

㝧ᴟ
㞟᮰㟁ᴟ

䜰䝹䝭䝙䜴䝮
ධຊ❆

ග㟁㠃
ධຊ⺯ග㠃

ධຊ㠃

⺯ග㠃ᇶ┙䠄䜰䝹䝭䝙䜴䝮䠅ᅗ㸲 ୰ᛶᏊ㹇㸬㹇㸬ࡢᵓ㐀ᅗ෭༷ᆺ䠟䠟䠠

䠏ᯈᘧ䠟䠟䠠䠟䠩䠫䠯ᅗ㸳 ྛ㏱㐣ീ෭༷ᆺ䠟䠟䠠

䠏ᯈᘧ䠟䠟䠠

ᅗ㸴 ྛ෌ᵓᡂ⏬ീ㻙㻌 㻟㻟㻠㻌㻙

䠟䠩䠫䠯

2-5

JAEA-Review 2011-050

2-6
㺀7179 ᳜≀ヨᩱ࡟࠾ࡅࡿỈศᕸゎᯒ㺁
Analysis of water distribution in plant tissue.
ᮾி኱Ꮫ኱Ꮫ㝔㎰Ꮫ⏕࿨⛉Ꮫ◊✲⛉      ୰す ཭Ꮚ◊✲ࡢ┠ⓗ࡜ព⩏ ᳜≀యࡢᐇ࡟ 9 ๭ࡣỈࡀ༨ࡵࠊ᳜≀࡟࠾ࡅࡿ࠶ࡽ
ࡺࡿ⏕⌮཯ᛂࡣỈ⁐ᾮ୰࡛⾜ࢃࢀࠊ᳜≀ࡢάືࡣỈࡢ፹௓↓ࡋ࡟ࡣ࠾ࡇࡾ࠼࡞࠸ࠋ≉࡟ࠊ㣴ศ྾཰ࡸ㣴ศࡢ㌿ὶ࡟࠾࠸࡚ࡣỈࡀ኱ࡁ࡞ᙺ๭ࢆᯝࡓࡋ࡚࠸ࡿ
ࡇ࡜ࡣ࿘▱ࡢ㏻ࡾ࡛࠶ࡿࠋ⏕ࡁࡓ᳜≀࡟࠾࠸࡚᭱ࡶ㔜せ࡞ᙺ๭ࢆᯝࡓࡋ࡚࠸ࡿ໬Ꮫ≀㉁ࡣఱ࡜࠸ࡗ࡚ࡶ
Ỉ࡛࠶ࡿ࡟ࡶ࠿࠿ࢃࡽࡎࠊỈࡑࡢࡶࡢࡢ▱ぢ࡟ࡘ࠸࡚ࡣ㠀ᖖ࡟ᑡ࡞࠸ࠋࡑࡇ࡛ᡃࠎࡣࠊ⏕ࡁࡓࡲࡲࡢ᳜
≀య୰ࡢỈࡢືࡁࡸศᕸࢆ᥈ࡿࡓࡵ࡟ࠊ୰ᛶᏊࣛࢪ
࢜ࢢࣛࣇ࢕࣮(NRG)ࢆ᥇⏝ࡋࠊỈ࡟≉␗ⓗ࡞ീࢆᚓࡿࡇ࡜ࢆ┠ⓗ࡟ᐇ㦂ࢆ㐍ࡵࡓࠋNRG ࡣṇ☜࡟ࡣỈ⣲ࡢീࡢྍど໬࡛࠶ࡿࡀࠊ᳜≀ヨᩱࡢỈ࡟ࡘ࠸࡚ヲ⣽࡟ㄪ࡭ࡿࡇ࡜ࡀ࡛ࡁࡿ᪉ἲࡣ NRG ࢆྵࡵᩘᑡ࡞࠸ࠋ
ヨᩱ࡜ࡋ࡚ࡣ࣐࣓⛉࡛༙஝⇱ᆅ࡟Ⰻࡃ⏕⫱ࡍࡿࠊ࢔ࢪ࢔ࠊ࢔ࣇࣜ࢝࡟࠾ࡅࡿ㔜せ࡞✐≀࡛࠶ࡿࢧࢧࢤ
ࢆ⏝࠸ࡓࠋࢧࢧࢤࡣࠊ᰿௜㏆࡟Ỉࡀ඲ࡃ࡞࠸≧ែࢆ
2 㐌㛫௨ୖ⥆ࡅ࡚ࡶࠊ෌ࡧỈࢆ୚࠼ࡿ࡜྾཰ࢆ㛤ጞࡋ⏕⫱ࢆ⥅⥆ࡍࡿࡇ࡜ࡀ࡛ࡁࡿ᳜≀࡛࠶ࡿࠋࡋ࠿ࡋࠊ
࡞ࡐࡇࡢࡼ࠺࡞ᙉ࠸஝⇱⪏ᛶ⬟ࢆಖᣢࡋ࡚࠸ࡿ࠿࡟
ࡘ࠸࡚ࡣ୙᫂࡞Ⅼࡀከ࠸ࠋࢧࢧࢤࡢⱼࡢ୍㒊࡟ࡣỈศྵ㔞ࡀ㧗࠸ࡶࡢࡀ࠶ࡾࠊࡇࡢ⤌⧊ࡀ㈓Ỉ⤌⧊࡜ࡋ࡚ᶵ⬟ࡋ࡚࠸ࡿࡽࡋ࠸࡜ゝࢃࢀ࡚࠸ࡿࡶࡢࡢࠊࡲࡔ
ᐇ㦂ⓗ࡟㈓Ỉ⤌⧊ࡢᶵ⬟࡟ࡘ࠸࡚☜࠿ࡵࡽࢀ࡚࠸࡞
࠸ࠋ஝⇱࡟ᙉ࠸࣓࢝ࢽࢬ࣒ࢆゎࡃࡓࡵ࡟ࡣࠊ஝⇱᫬ࡢ᳜≀యෆỈศᕸࢆヲ⣽࡟ᢕᥱࡍࡿᚲせࡀ࠶ࡿࠋᮏ
◊✲࡛ࡣࠊNRG ࢆ⏝࠸࡚ࠊ᳜≀యෆỈศศᕸࢆゎᯒࡋࡓࠋࡑࡢ◊✲ࢆ࡝ࡢࡼ࠺࡟⾜ࡗࡓ࠿ ᮏ◊✲࡛ࡣࠊ࢔ࣇࣜ࢝ࡢ஝⇱ᆅᇦ࡛⮬⏕ࡋ࡚࠸ࡿࢧࢧࢤ⣙ 2000 ✀࠿ࡽ㑅ᢤࡉࢀࡓ஝⇱࡟⪏ᛶ࡞ရ✀࡜஝⇱࡟ឤཷᛶ࡞ရ✀ࢆ⏝࠸ࡓࠋලయⓗ࡟ࡣࠊ஝⇱⪏ ᛶ ရ ✀ ࡢ ࢧ ࢧ ࢤ 2 ရ ✀ ࠊ Vigna unguiculata
TVu11979, TVu11986 ࡜ࠊ஝⇱ឤཷᛶရ✀ࡢࢧࢧࢤ 2
ရ✀ Vigna unguiculata TVu7778ࠊTVu9357 ࢆ౑⏝ࡋࡓࠋ✀Ꮚ⾲㠃࡟ࣖࢫ࡛ࣜയࢆࡘࡅࡓᚋࠊỈ㐨Ỉ࡛‵ࡽࡏࡓࣂ࣮࣑࢟ࣗࣛ࢖ࢺ࡬᧛✀ࡋࠊᬯᡤ࡟࠾࠸࡚
30Υ࡛ 2 ᪥㛫ฎ⌮ࡋⓎⱆࡉࡏࡓࠋⓎⱆᚋࠊ5 ᪥㛫
1/4Hogland Ỉ⪔ᾮ࡛⏕⫱ࡉࡏࠊࡑࡢᚋ᧛✀ᚋ 24 ᪥┠ࡲ࡛ Hogland Ỉ⪔ᾮ࡛⏕⫱ࡉࡏࡓࠋỈ⪔ᾮࡣ 7 ᪥ẖ࡟ ஺ ᥮ ࡋ ࡓ ࠋ ⏕ ⫱ ⎔ ቃ ࡣ ே ᕤ Ẽ ㇟ ჾ (BIOTRON
LPH300:NK system Co. Japan)ෆ࡛ ᗘ 28Υࠊ‵ᗘ
70㸣ࠊ᫂ᮇ 16 hࠊᬯᮇ 8 hࠊග᮲௳ 150 ȣmolm-2sec-1
࡜ࡋࡓࠋ୍᪉ࡢࢧࣥࣉࣝࡣᘬࡁ⥆ࡁᨵⰋ Hogland Ỉ⪔ᾮ࡛ 3 ᪥㛫⏕⫱ࡉࡏࠊ௚᪉ࢆ 3 ᪥㛫஝⇱ࢫࢺࣞࢫฎ⌮ࡋࡓ(஝⇱ࢫࢺࣞࢫᮇ㛫୰ࡢ‵ᗘࡶ 70㸣࡜ࡋࡓ)ࠋ
NRG ࡢ᧜ᙳࡣࠊ᪥ᮏཎᏊຊ◊✲㛤Ⓨᶵᵓࠊᮾᾏ◊✲ᡤࡢ◊✲⏝ཎᏊ⅔ࠊFRR3 ࢆ⏝࠸࡚⾜࡞ࡗࡓࠋ୰
ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ᑓ⏝ࡢ୰ᛶᏊ⥺ྲྀࡾฟࡋཱྀ࡟࠾
ࡅࡿ⇕୰ᛶᏊ᮰ࡣࠊ1.5㹶108n/cm2/s ࡛࠶ࡿࠋཎᏊ⅔
࠿ࡽࡢ୰ᛶᏊ⥺࡟ࡼࡿ↷ᑕീࡣࠊ55 mm ࣞࣥࢬ(✵㛫ศゎ⬟ 200 ȣmࠊど㔝 20 cm20 cm)࡟ࡼࡾࠊ5 ᯛࢆ
1 ࢭࢵࢺ࡜ࡋ࡚᧜ᙳࡋࡓࠋ◊✲ᡤෆࡢᐊ ࡣ 20Υࠊ‵ᗘ 27㸣࡛࠶ࡾࠊ᧜ᙳᐊࡣᐊ 28Υࠊ‵ᗘ 22㸣࡛࠶ࡗࡓࠋࡲࡓࠊ᧜ᙳ୰ࠊ௚ࡢࢧࣥࣉࣝࡣேᕤẼ㇟ჾෆ࡛ ᗘ 28Υࠊ‵ᗘ 70㸣ࠊ᫂ᮇ 16 hࠊᬯᮇ 8 hࠊග᮲௳ 150 ȣmolm-2sec-1 ࡟ಖࡗࡓࠋ᧜ᙳ㛤ጞ๓࡟ࡣ
CCD ࣓࢝ࣛࡢᬯ㟁ὶ⏬ീ࡜ࢧࣥࣉࣝࢆ⨨࠸࡚࠸࡞࠸≧ែ࡛ࡢ NRG ⏬ീ(ࣂࢵࢡࢢࣛ࢘ࣥࢻ⏬ീ)ࢆ᧜ᙳ
ࡋࡓࠋ஝⇱ࢫࢺࣞࢫ๓࣭ࢫࢺࣞࢫᚋࡑࢀࡒࢀࠊࢧࢧࢤ 4
ရ✀ࠊ3 㐃࡛᧜ᙳࡋࡓࠋ5 ᯛࡢ⏬ീࢭࢵࢺࢆ 1 ᯛࡢ⏬
ീ࡟⤫ྜࡋ㸦᧜ᙳࡋࡓ 5 ᯛࢭࢵࢺࡢ⏬ീࡢࣆࢡࢭࣝ
ࡈ࡜ࡢ᭱ప್ࢆ࡜ࡾࠊ1 ᯛࡢ⏬ീ࡬ኚ᥮ࡋࡓ㸧ࠊᬯ㟁ὶ⏬ീ࡜ࣂࢵࢡࢢࣛ࢘ࣥࢻ⏬ീࢆ⏝࠸࡚᳜≀యࡢ୰ᛶᏊ⥺㏱㐣⏬ീࢆᚓࡓࠋࡇࡢ⏬ീࡣ୰ᛶᏊ⥺ࡀ㏱㐣ࡍࡿ࡯࡝᫂ࡿࡃࠊῶ⾶ࡍࡿ࡯࡝ᬯࡃ෗ࡗ࡚࠾ࡾࠊỈศྵ㔞ࡢከ࠸࡜ࡇࢁ࡯࡝⃰ࡃ෗ࡗ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋࡲࡓࠊ2 ḟඖࡢ NRG ⏬ീ࡜ࡣู࡟ 3 ḟඖ NRG ⏬
ീࡶ᧜ᙳࡋࡓࠋࡇࡢᐇ㦂ࡣ TVu7778 ࡜ TVu11979 ࡟ࡘ࠸࡚ࠊ஝⇱ฎ⌮ࡢ᭷↓ࡑࢀࡒࢀ࡟ 2 㐃࡛⾜ࡗࡓࠋ᧛✀ᚋ 19 ᪥┠ࡢࢧࣥࣉࣝ࡜ࠊ᧛✀ᚋ 19 ᪥┠࠿ࡽ஝    JRR3 NRG  ᳜≀ヨᩱ࡟࠾ࡅࡿỈศᕸゎᯒ㻙㻌 㻟㻟㻡㻌㻙

JAEA-Review 2011-050⇱ࢫࢺࣞࢫ᮲௳ୗ࡟ 8 ᪥㛫ࡉࡽࡋࡓࢧࣥࣉࣝ࡜ࢆẚ㍑ࡋࡓࠋࢧࣥࣉࣝࡣ➨୍ⴥࡢⴥ᯶ୗ 6 cm ࡢ㒊ศ(ึฟⴥୗ 1 cm ⛬ᗘࡲ࡛࡟࠶ࡓࡿ)ࡢⱼࢆษࡾࡔࡋࠊ࢔
࣑ࣝ࣍࢖ࣝ࡟ໟࢇ࡛෇ᰕ≧࡟ຍᕤࡋࡓࠋ┤ᚄ 1 cm ࡢ࢔࣑ࣝ〇ࡢ෇ᰕ࡬ࢧࣥࣉࣝࢆᅛᐃࡋࠊ200 mm ࣞࣥࢬ(✵㛫ศゎ⬟ 50 ȣmࠊど㔝 5 cm5 cm)ࢆ⏝࠸࡚ࠊࢧࣥࣉࣝࢆ 0.5 ᗘࡎࡘ 180 ᗘᅇ㌿ࡉࡏࠊྛᅇ㌿ゅᗘ࡟࠾࠸࡚ NRG ⏬ീࢆ᧜ᙳࡋࡓࠋྲྀᚓࡋࡓ 360 ᯛࡢ⏬ീࢆ IPLab(Scanalytics,Inc.)࡟ࡼࡗ࡚ฎ⌮ࡋࠊ3 ḟඖ
NRG ⏬ീ࡜ࡋ࡚ᵓ⠏ࡋࡓࠋࡲࡎࠊ⏬ീࢆᶓ᪉ྥ࡟㍯
ษࡾ࡟ࡋࠊ࡛ࡁࡓᖜ 1 ࣆࢡࢭࣝࡢ⣽ษࢀࡢ⏬ീࢆࡑࢀࡒࢀ⏬ീࡢᶓᖜศࡢࣆࢡࢭࣝᩘࡔࡅ୪࡭ࡓࠋࡇࡢ
ṇ᪉ᙧࡢ⏬ീࢆྛゅᗘ࡛᧜ᙳࡋࡓ⏬ീࡈ࡜࡟సࡾࠊ
࠾ࡢ࠾ࡢࡢゅᗘศᅇ㌿ࡉࡏࠊ඲࡚ 1 ᯛ࡟㊊ࡋྜࢃࡏࡓࠋࡇ࠺ࡋ࡚ฟ᮶ࡓ⏬ീ࡟ࣇ࣮࢚ࣜኚ᥮ࣀ࢖ࢬ㝖ཤࢆ⾜࠸ࠊ1 ᯛࡢ᩿㠃ീ࡜ࡋࡓࠋࡑࡋ࡚ࠊࡇࡢ᩿㠃ീ
ࢆ᭱ึ࡟㍯ษࡾ࡟ࡋࡓྛ⏬ീศ୪࡭ࡿࡇ࡜࡛ࠊ3 ḟ
ඖ NRG ീࢆ෌ᵓ⠏ࡋࡓࠋ

᪂ⱆ
➨୕ⴥ

➨ᅄⴥ(a
ⴥ)
➨஧ⴥ(cⴥ)

(bⴥ)
➨୍ⴥ
(dⴥ)

Fig. 2-1䠖䝃䝃䝀஝⇱ឤཷᛶရ✀䛾NRGീ
ᕥୖ䠖TVu7778஝⇱䝇䝖䝺䝇๓ྑୖ䠖TVu7778஝⇱䝇䝖䝺䝇ᚋᕥୗ䠖TVu9357஝⇱䝇䝖䝺䝇๓ྑୗ䠖TVu9357஝⇱䝇䝖䝺䝇ᚋ

ึฟⴥ
Ꮚⴥ⑞

Fig1䠖 䝃䝃䝀(Vigna unguiculata L. Walp.)࡝ࡢࡼ࠺࡞⤖ᯝࢆᚓࡓ࠿ ࢧ ࢧ ࢤ ࡢ஝ ⇱ ឤ ཷ ᛶရ ✀ ࠊ TVu7778 ࡞ ࡽ ࡧ ࡟
TVu9357 ࡟ࡘ࠸࡚ࠊ஝⇱ࢫࢺࣞࢫࢆ୚࠼ࡿ๓࡜ᚋ࡟
࠾࠸࡚ NRG ᧜ᙳࢆ⾜࡞ࡗࡓࠋࡑࡢ⤖ᯝࢆ Fig. 2-1 ࡟♧ࡋࡓࠋࡲࡓࠊ஝⇱⪏ᛶရ✀ࠊTVu110979 ࡞ࡽࡧ࡟TVu 11986 ࡟ࡘ࠸࡚ࡢ NRG ീࢆ Fig. 2-2 ࡟♧ࡋࡓࠋࡲࡎࠊ஝⇱⪏ᛶࡢရ✀㸦Fig. 2-2㸧ࡢ᪉ࡀࠊ஝⇱ฎ⌮๓ᚋ࡟࠾ࡅࡿᙧែࡸỈศྵ㔞ࡢᕪࡀᑡ࡞࠸ࡇ࡜ࡀ♧ࡉࢀࡓࠋ

ࡉࡽ࡟ヲ⣽࡟ᚓࡽࢀࡓീࢆࡳ࡚ࡳࡿ࡜ࠊ≉࡟஝⇱⪏ᛶရ✀࡟࠾࠸࡚ࡣࠊ➨୍ⴥ࠿ࡽ➨୕ⴥࡢ㛫ࡢⱼ⠇㸦Fig. 1 ཧ↷㸧ࡢỈศྵ㔞ࡀ㧗࠸ഴྥࡀぢࡽࢀࡓ(⃰࠸ᙳࡀぢࡽࢀࡓ)(Fig. 2-1ࠊ2-2)ࠋࡲࡓࠊ㏻ᖖࡢ⎔ቃ᮲௳ୗ࡛ࡣࠊࡇࡢⱼࡢ㒊఩࡟Ỉࡀከࡃྵࡲࢀ࡚࠸ࡿࡇ
࡜ࡀࢃ࠿ࡗࡓࠋ஝⇱ࢫࢺࣞࢫฎ⌮ࢆ࠿ࡅࡿ࡜ࠊࡍ࡭
࡚ࡢရ✀࡟࠾࠸࡚ࠊୗࡢⴥ࠿ࡽỈศࡀῶᑡࡋ࡚࠸ࡃ
ᵝᏊࡀ♧ࡉࢀࡓࠋࡋ࠿ࡋࠊ஝⇱⪏ᛶရ✀࡛ࡣ≉࡟ⴥ࠿ࡽࡢỈศῶᑡࡀᑡ࡞࠸ࠊࡘࡲࡾⴥࡀᯤࢀ࡟ࡃ࠸ࡇ
࡜ࡀࢃ࠿ࡗࡓࠋ஝⇱⪏ᛶရ✀࡜ឤཷᛶရ✀ࢆẚ㍑ࡍ
ࡿ࡜ࠊ஝⇱⪏ᛶရ✀ࡣࠊឤཷᛶရ✀ࡼࡾࡶⱼ୰ࡢỈྵ㔞ࡀಖࡓࢀ࡚࠸ࡿࡇ࡜ࡶ♧ࡉࢀࡓࠋࡇࢀࡽࡢࡇ࡜
࠿ࡽࠊ஝⇱⪏ᛶရ✀ࡣࠊⴥࢆ࡞ࡿ࡭ࡃᯤࡽࡏ࡞࠸ᶵ
ᵓࠊࡘࡲࡾ஝⇱᫬࡟ⴥࢆಖᣢࡍࡿᶵᵓ࡜ࡋ࡚ࠊⱼࡢỈྵ㔞ࢆ࠶ࡲࡾῶࡽࡉ࡞࠸ᶵᵓ࡜ࠊⴥ࡜ⱼࡑࢀࡒࢀ࡟஝⇱⪏ᛶ࡟ᐤ୚ࡍࡿᶵᵓࡢᏑᅾࡀ♧၀ࡉࢀࡓࠋ≉࡟ࠊ஝⇱⪏ᛶရ✀࡛ࡣࠊⱼࡀኴࡃࠊྵỈ⋡ࡶ㧗࠸ࡇ࡜࠿ࡽࠊࡇࡢ㒊఩ࡀ஝⇱᫬࡟Ỉࡢ౪⤥ඖ࡜ࡋ࡚ᐤ୚
ࡋ࡚࠸ࡿࡇ࡜ࡀண᝿ࡉࢀࡿࠋࡉࡽ࡟ࠊⴥࡶᯤࢀ࡟ࡃ
࠸ࡇ࡜࠿ࡽࠊỈࡀⱼ࠿ࡽⴥ࡬⛣⾜ࡋ⵨Ⓨࡋ࡚ኻࢃࢀ
ࡿࡇ࡜ࡀ࡞࠸ࡼ࠺࡞࣓࢝ࢽࢬ࣒ࡀാ࠸࡚࠸ࡿࡇ࡜ࡀ
⪃࠼ࡽࢀࡓࠋ
2-6

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JAEA-Review 2011-050

Fig. 2-2䠖䝃䝃䝀஝⇱⪏ᛶရ✀䛾NRGീ
ᕥୖ䠖TVu11979஝⇱䝇䝖䝺䝇๓ྑୖ䠖TVu11979஝⇱䝇䝖䝺䝇ᚋᕥୗ䠖TVu11986஝⇱䝇䝖䝺䝇๓ྑୗ䠖TVu11986஝⇱䝇䝖䝺䝇ᚋ

Fig. 3䠖ⱼ(ึฟⴥ௜䛡᰿)䛾❧యⓗNRG⏬ീᕥୖ䠖TVu7778஝⇱䝇䝖䝺䝇๓ྑୖ䠖TVu7778஝⇱䝇䝖䝺䝇ᚋᕥୗ䠖TVu11979஝⇱䝇䝖䝺䝇๓ྑୗ䠖TVu11979஝⇱䝇䝖䝺䝇ᚋḟ࡟ࠊࢧࢧࢤࡢ⠇ࡢ 3 ḟඖ NRG ⏬ീࢆ᧜ᙳࡋࡓࠋ
ࡑࡢ⤖ᯝࠊ஝⇱ࢫࢺࣞࢫ࡟ࡼࡗ࡚ⱼ⠇ࡢỈศࡶᢤࡅࡓࡇ࡜ࡀ☜ㄆ࡛ࡁࡓࠋࡋ࠿ࡋࠊ஝⇱⪏ᛶရ✀ࠊឤཷᛶရ✀࡜ࡶ࡟ྠᵝ࡟ⱼ⠇ࡢỈࡣኻࢃࢀ࡚࠸ࡓࠋ௒ᅇ
ࡢ≧ἣࡲ࡛஝⇱ࡉࡏ࡚ࡶࠊỈࢆ෌ᗘ୚࠼ࡿ࡜⏕⫱ࡀᅇ᚟ࡍࡿࡇ࡜࠿ࡽࠊⱼ⠇ࡢỈࡀ࡞࠸஝⇱≧ἣ࡛ࡶ㝆㞵➼࡛⏕⫱ࡀᅇ᚟ࡍࡿ㝿࡟ࡣࠊ⠇㒊఩࡟Ỉࡀ౪⤥ࡉࢀࡿࡇ࡜ࡀุ᫂ࡋࡓࠋࡋ࠿ࡋࠊࡑࡢ㝿࡟Ỉ౪⤥ᶵᵓࡣ୙࡛᫂࠶ࡗࡓࠋࡲࡓࠊࡇࡢ⪏ᛶᶵᵓࡣࢧࢧࢤ࡜ࡋ
࡚ಖ᭷ࡋ࡚࠸ࡿࡶࡢ࡛࠶ࡾࠊࢧࢧࢤࡢရ✀㛫ᕪ࡟ᐤ୚ࡍࡿࡶࡢ࡛ࡣ࡞࠸ࡇ࡜ࡀண᝿࡛ࡁࡓࠋ
ࡑࡢ⤖ᯝ࡟ᑐࡍࡿホ౯᳜≀య୰࡟ྵࡲࢀࡿỈࡢ࢖࣓࣮ࢪࣥࢢᡭἲ࡜ࡋ࡚
୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ࢆ⏝࠸ࡓࠋ୰ᛶᏊࣛࢪ࢜ࢢࣛ
ࣇ࢕ࡣᑐ㇟≀࡟୰ᛶᏊ⥺ࢆ↷ᑕࡋ࡚୰ᛶᏊ⥺ࡢ㏱㐣⏬ീࢆᚓࡿᡭἲ࡛࠶ࡿࠋ୰ᛶᏊ⥺ࡢῶ⾶ཎᅉ࡜ࡋ࡚ࠊ
᳜≀యෆ࡛ࡣࡑࡢᏑᅾ㔞࠿ࡽࡶ H2O ࡢᙳ㡪ࡀᴟࡵ࡚኱ࡁ࠸࡜⪃࠼ࡽࢀࡿࡇ࡜࠿ࡽࠊ᳜≀యෆࡢỈศྵ㔞ࢆ㠀◚ቯⓗ࡟ ᐃ࡛ࡁࡿ᭷ຠ࡞᪉ἲ࡛࠶ࡿࠋ

ᮏ◊✲⤖ᯝࡣࠊࢧࢧࢤࡢ⪏ᛶ࣓࢝ࢽࢬ࣒ࢆゎ᫂ࡍࡿ┠ⓗ࡛ࠊࢧࢧࢤయෆࡢỈศྵ㔞࠾ࡼࡧ஝⇱᫬ࡢỈศศᕸࢆゎᯒࡋࡓࠋࡑࡢ㝿࡟ࡣࠊ3D ࡟ࡼࡿ᧜ᙳ࡟ᣮ
ᡓࡋࠊⱼ⠇㒊఩࡛ࡢヲ⣽࡞Ỉศᕸࡀ᫂ࡽ࠿࡜࡞ࡗࡓࠋ
ᮏ◊✲࡛ᚓࡽࢀࡓ⠇㒊఩࡛ࡢỈྵ㔞ኚ໬ࡣࠊࢧࢧࢤ
⪏ᛶ࣓࢝ࢽࢬ࣒ࢆゎ᫂ࡍࡿ࡟࠶ࡓࡾ㈗㔜࡞▱ぢ࡛࠶ࡿࠋ࡜࠸࠺ࡢࡶࠊ୍᪦Ỉࡀᢤࡅࡓ⤌⧊࡟Ỉࢆ౪⤥ࡍࡿࠊ࡜࠸࠺௙⤌ࡳࡣ᳜≀࡟࡜ࡗ࡚࡜࡚ࡶ࢚ࢿࣝࢠ࣮ࡢせࡿసᴗ࡛࠶ࡾࠊࢧࢧࢤࡢⱼ⠇㒊఩࡛ࡑࡢࡼ࠺࡞
⾜ືࢆ࡜ࡗ࡚࠸ࡿࡇ࡜ࡣࠊ஝⇱⪏ᛶᶵᵓ࡟ⱼ⠇㒊఩ࡀ㔜せ࡛࠶ࡿࡇ࡜ࢆ♧၀ࡋ࡚࠸ࡿࠋࡉࡽ࡞ࡿ▱ぢࢆᚓࡿ࡟ࡣࠊ෌ᗘỈࢆ౪⤥ࡋࡓሙྜࡢࢧࢧࢤ⠇㒊఩ࡢỈศᕸࢆ᧜ᙳࡋࡓࡾࠊࡼࡾᐃ㔞ⓗ࡞ࢹ࣮ࢱࢆ♧ࡏࡿࡼ࠺࡞ゎᯒࢆ⾜࠺ᚲせࡀ࠶ࡿࡶࡢ࡜ᛮࢃࢀࡿࠋ
ᡂᯝࡢබ⾲ᮏ◊✲ᡂᯝ࡟ࡘ࠸࡚ࡣࠊᏛ఍Ⓨ⾲➼࡛ࡣබ⾲ࡋ࡚࠾
ࡾࡲࡏࢇ
2-6

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3.  හ⊒ࠟࡦࡑ✢ಽᨆ 

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JAEA-Review 2011-050

3-1Development of a Method of Measuring the Cadmium Concentrationin Agricultural Produce with Prompt γ-ray Analysis
Y. Sakurai1 , H. Matsue2 , S. Miyamoto1 and N. Kihou1
1

National Institute for Agro-Environmental Sciences, Tsukuba, Ibaraki 305-8604
2
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

1. Objective
Enhancement of regulations on standard
levels of cadmium in foods is currently being
studied both here in Japan and abroad. The
most eﬀective way of ensuring risk management of the cadmium concentration in agricultural produce and animal feed is to monitor the cadmium concentration in produce.
Thus, we developed a method of measuring the cadmium concentration in agricultural
produce and animal feed with PGA, which
is a method of non-destructive analysis that
does not require wet decomposition of samples, in order to measure cadmium concentrations rapidly and with a high level of accuracy.
In 2007, we studied the eﬀects of noise level
attenuation and sample form on measurement
accuracy in order to improve the sensitivity of
cadmium detection.

Table 1: Thickness of the acrylic sheet ﬁlter and the
S/N ratio of Cd in brown rice

Acrylic sheet
thickness (mm)02
3
5

S/N ratio of the
Cd peak
0.121 ± 0.022
0.199 ± 0.012
0.179 ± 0.002
0.0788 ± 0.015

Table 2: Sample form and S/N ratio of Cd in brownriceForm of brown rice
samplePellets(6.1g)
Powder(5g)Grains(5g)S/N ratio of the
Cd peak
0.0529 ± 0.0065
0.0446 ± 0.0039
0.0315 ± 0.0003

2. Methods
An acrylic sheet (150 mm x 150 mm, d=2,
3, or 5 mm) was inserted as a noise ﬁlter in aneutron beam line prior to samples being analyzed with a PGA device, and the S/N ratio of
the prompt γ ray peak (558 keV) of cadmiumin brown rice (Cd: 2 μg/g) was measured for1500 s. In addition, ground samples (5-6 g)of brown rice (Cd: 0.6 μg/g) were placed inaluminum rings and shaped into round pellets(Φ40 mm) with a hydraulic press (20t/cm2 ),and the S/N ratio of the cadmium peak ofthese samples was compared to that of powdered and granular samples of brown rice.
3. Results
Eﬀects of the insertion of an acrylic sheet in
the beam line on cadmium measurements inbrown rice are shown in Table 1, and eﬀects
of diﬀerent forms of samples on the S/N ratioof cadmium are shown in Table 2.
原子炉：JRR-3

装置：PGA(T1-4)

4. Discussion/Conclusion
Results of placing an acrylic sheet in theneutron beam and measuring the Cd peak inbrown rice indicated that the S/N ratio improved about 1.5-fold when an acrylic sheetwith a thickness up to 3 mm was inserted in
the beam line. The sheet’s eﬀect, however,
was limited, so the same measurements weremade the following year as well. The sample
form had an eﬀect on the S/N ratio in theorder of shaped pellets>powder>grains; thisis believed to be the order of greater brownrice sample density in the neutron beam’s target plane. Even when brown rice powder was
molded into shape, doing so improved the S/Nratio of the powdered sample only 1.2-fold, so
measured with a powdered sample is recommended because of its analysis eﬃciency.

分野：即発γ線分析実験（農・水産物）

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JAEA-Review 2011-050

3-2
Measurements of Hydrogen-Containing Samples Using MPGA
Y. Toh, M. Oshima, M. Koizumi, K. Furutaka, A. Kimura and Y. Murakami1
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195
1
JST Innovation Satellite Ibaraki, JST, Tsukuba, Ibaraki 305-0047

Many of agricultural, medical and industrial samples contain large amounts of hydrogen. Hydrogen emits a 2.2MeV prompt
gamma ray in a neutron capture reaction.
The low-energy photons due to the Compton scattering of high energy γ rays fromhydrogen obviously cause an increase in the
background in the lower region of the γ spectrum, resulting in a decrease in the detection
limit. Hydrogen emits only one prompt γ ray
at a time at every neutron capture reaction.
The multiple γ-ray detecting method, which
is known as a coincidence method, is widelyused in nuclear spectroscopy. In this method,
only elements which simultaneously emit two
or more prompt gamma ray in a capture reaction can be measured 1, 2) . Therefore, by applying the multiple γ-ray detection method
to PGA, the inﬂuence from hydrogen can be
reduced.
A standard polymer sample (IRMM
BCR681) which contain 22 ppm Cd wasmeasured by the MPGA detector system.
The event rate was about 220k count/sec.
Cadmium emits some prompt γ rays mainlyin the neutron capture reaction of 113 Cd(n,1) Y.Toh, et al. :“Appl. Radiat. Isotopes”, 64, pp.
751-754 (2006).
2) M.Oshima , et al. :“Proc. J. Radioanal. Nucl.
Chem.”, 271, 317 (2007).

a) PGA

4
3
2

Cd
H

[×10 ]

1
0
0

1
0.8

CountsCountsReferences

55[×10 ]γ)114 Cd: 558-, 576-, 651- and 725-keV γrays, for example. PGA and MGPA spectrum were compared in the Fig.1. In ﬁg.1,
the normalized projection spectra of thetwo-dimensional spectra with change in thescaling of the Y axis is shown for comparison.
In the MPGA spectrum, hydrogen peak was
reduced and signal-to-noise ratio of Cd was
improved.
Polymer standard samples BCR680, B7
and a standard rice sample NIES CRM No.10
were also measured by the MPGA detector system. These samples contain diﬀerent
amounts of cadmium (BCR680 141 ppm , B7
4.8 ppm, CRM No.10 1.8 ppm) . A calibration curve for quantiﬁcation of cadmium was
obtained. The cadmium calibration curve exhibited good linearity in the range of 1.8 to141ppm.
This research was partly conducted as
the Practical Application Research and supported by JST Innovation Satellite Ibaraki.

0.6

Cd

0.4
0.2
0
0

1000
2000
Energy (keV)b) MPGA

H
1000
2000
Energy (keV)

Figure 1: a) PGA and b) MPGA spectrum for a standard polymer sample (IRMM BCR681). The normalized
projection spectra of the two-dimensional spectra with a change in the scaling of the X axis is shown forcomparison to the PGA spectra.

原子炉：JRR-3

装置：MPGA(C2-3-2)

分野：即発γ線分析実験（農・水産物）

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JAEA-Review 2011-050

3-3
Determination of Boron in Ceramic Reference Materials by Prompt Gamma-ray
Analysis Using Focused Neutron Guided Beam of JRR-3M
T. Miura1 , H. Matsue2 , T. Kuroiwa1 and K. Chiba1
1

2

N ationalM etrologyInstituteof Japan − AIST, Ibaraki305 − 8563
QuantumBeamScienceDirectorate, JAEA, T okai, Ibaraki319 − 1195

Prompt gamma-ray analysis (PGA) is useful for nondestructive determination of lightelements such as B in bulk samples. However, a long counting time is generally required to measure suﬃcient gamma ray spectrum by straight neutron beam irradiation.
Recently, a new beam focusing unit for JRR3M was developed which increases beam ﬂux
increase by 3 times−1 )1,) . However, the proﬁle of the focused neutron beam is usuallyless homogeneous than when compared with astraight neutron beam. Appropriate internal
standards are required to correct the inhomogeneity of neutron ﬂux and make the irradiation uniform enough for precise and accurate
determination. The aim of this study was toevaluate the analytical performance of PGA
using the focused neutron beam. The PGA
was applied to the determination of B in SiC
ceramics CRM (BAM S-003), and the eﬀect
of an internal standard and the measurement
uncertainty in PGA were investigated.
The B standards were prepared from NMIJ
primary standard solution. A series of B standards (0, 1.2, 4.7 and 10.6 ug of B) were prepared, each of which contained Si metal and
ND4Cl as matrices. Another aliquot of 25 mg
of ND4Cl was weighed and put into another
FEP ﬁlm bag to prepare the ND4Cl standard
sample, which was used to measure the correction factor to correct the spectral interference. Three aliquots of 100 mg of BAM S-003
were weighed and put into the FEP ﬁlm bags.
The FEP ﬁlm bags were heat-sealed to makethe sample packages smaller than 15 mm x 15
mm. The blank levels of B in Si metal and
ND4Cl had been measured by the PGA andwere less than 0.3 ug both in 250 mg of Si
metal and 25 mg of ND4Cl. The samples andstandards were irradiated by the focused neu原子炉：JRR-3

装置：PGA(T1-4)

tron beam at JRR-3M. The prompt gamma
ray spectrum was measured with Compton
suppression PGA system for 1000 to 8000 s
according to the spectrum intensity. The B
gamma ray peaks were analyzed by Covells method and by the non-linear least squares
method2) . The determination of B was carried out by linear calibration curves using aninternal standard. The Cl 1601 keV peaks
were used as an internal standard. The analytical result of B in BAM CRM S003 (63.3
mg/kg ± 3.0 mg/kg, k =2)3) is in good agreement with the certiﬁed value (63 mg/kg ±7 mg/kg, k =2) which was characterized by
the analytical results obtained by ICP-OES,
DCarc-OES and molecular absorption spectrometry. The main component of the standard uncertainty was the sample measurement repeatability for BAM CRM S-003.
PGA using the focused neutron beam wasapplied to the determination of B in ceramic
CRM. The internal standard method wasfound to be useful for the focused neutron
beam irradiation method. PGA using the focused neutron beam can be determined in therange of 0 to 10 ug of B in ceramics sample
without any sample dissolution.
References
1) S. Yamada et al :“Physica B”, 385-386, 1243(2006).
2) M. Magara and C. Yonezawa :“Nucl. Instr. andMeth”,A454, 389(2000).
3) CRM BAM-S003 Certiﬁcate :Federal Institute forMaterial Research and Testing, BAM, Berlin, 2004.

分野：即発γ線分析実験（工業材料）

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JAEA-Review 2011-050

3-4
Non-Destructive Analysis of Ancient Egyptian Vitreous Relics by Neutron
S. Yoshida
Department of Energy Science and Technology, Tokai University, Kanagawa 259-1292

On our laboratory, ancient Egyptian vitreous relics (faience) and sand or rock which become those raw materials are analyzed by thenon-destructive simultaneous multi-elements
measurement using the prompt gamma-ray
analysis (PGA) by neutron beam, because itis extremely a very small amount of the residual radioactivity after irradiation when neutron ﬂux is low. Our goal in this study is
to examine what archeological characteristics
in those distributions of some component elements of main elements and trace elements
speciﬁed exist, such as times nature and regional nature. The analysis has been carriedout by the thermal neutron prompt gammaray analysis used the T1-4-1 beam port of
the JRR-3 institution. Many analysis samples were faience of ancient Egyptian vitreous relics or sand and rock of the orient area,
many samples of about 5cm x 10cm at the
maximum (thickness a little less than 1cm)
were sealed up with an FEP ﬁlm individually,
and analyzed while irradiating it by 3,0005,000 seconds per one sample on the sample
stage center in the whole He-gas atmosphere
after a set. The relations with Fe/Si ratio(ratio of the peak area net count rate of the
full-energy peak of Fe (E γ=352keV) for theone of Si (E γ=3539keV) which is a main element) and Co/Si ratio (mainly, the Nile central part, the Akoris remains) in each faienceand local sand, were shown in Fig. 1. We havebeen investigated that Fe ratio in sand (Si)was strongly proportional related to Co ratio,
however, could not ﬁnd a regional characteristic. In addition, it follows that the existence
ratio between each element in faience accords
with the one in sand. But it is consideredthat cobalt was elemental addition at the timeof faience production and it was showed topresent distribution that it came oﬀ from existence distribution of the sand (inside pointsof the dotted line in Fig. 1). Furthermore,
原子炉：JRR-3

装置：PGA(T1-4)

the existence ratio distribution with Co element and Cu element which it was detectedin faience without it being detected into sandwas shown in Fig.2. By the distribution thatthe existence ratio of the Co and Cu become
1 as for the dotted line crossing the center atthe opposite angle, it has been revealed thattwo groups formed characteristic distributionthat the upper domain where the existence
ratio of the Cu is big in comparison with the
Co and the lower domain where the existence
ratio of the Cu is small.

Figure 1: Comparison of the existence ratio of Fe andCo in faience and sand.

Figure 2: Comparison of the existence ratio of Co and
Cu in faience.

分野：即発γ線分析実験（考古学）㻙㻌 㻟㻠㻠㻌㻙

JAEA-Review 2011-050

3-5Development of Temperature Variable Neutron In-beam Mössbauer
Spectrometer
M. K. Kubo, Y. Kobayashi1 , Y. Yamada2 , Y. Watanabe3 , T. Takayama3 Y. Sakai3 , H. Shoji4 ,W. Sato5 , A. Shinohara5 , M. Segawa6 , H. Matsue6
Department of Chemistry, International Christian University, Tokyo 181-8585
1
Applied Nuclear Physics Laboratory, RIKEN, Saitama 351-0198
2
Department of Chemistry, Tokyo University of Science, Tokyo 162-8061
3
Daido Institute of Technology, Nagoya 457-8530
4Graduate School of Science, Tokyo Metropolitan University, Tokyo 192-0039
5
Department of Chemistry, Graduate School of Science, Osaka University, Osaka 560-0043
6
Japan Atomic Energy Agency, Ibaraki 319-1195

原子炉：JRR-3

装置：PGA(T1-4)

of material hit by the beam while keeping thevacuum of the cryostat.
At room temperature the neutron in-beam
Mossbauer spectrum of pyrite was composedof two doublets. At 78K the spectrum of
pyrite was decomposed into three doublets(Figure 1). Component A had similar Mossbauer parameters as the parent pyrite. Doublet B showing IS=0.08(5) mms−1 and QS= 1.0(1) mms−1 could be Fe(III) in low spinstate, and doublet C with IS=0.68(8) mms−1
and QS = 1.27(13) mms−1 might be Fe(II)in high spin state. At this point we cannot determine the details of these two new
species. But it could safely be said that the
spectrum at low temperature is diﬀerent fromthe one at room temperature and more than
two species appeared in the spectrum might
be attributable to species produced by the nuclear event but could not be observed at room
temperature due to their thermal instability.
RT
105

Relative intensity

Emission Mössbauer spectroscopy is a useful tool in the investigation of the trace
amount of chemical species formed by nuclear reactions and radioactive decays. The
large transmission power of γ-ray used by
the Mössbauer eﬀect enables non-destructive
analysis of the inside of solid materials inwhich nuclear events occur. We have been developing a new 57 Fe in-beam Mössbauer spectroscopic system in order to investigate thechemical and physical behaviors of the species
produced after the neutron capture reactionof 56 Fe in materials. This year we introduced
a liquid N2 cryostat to try freezing and keeping thermally unstable initial nuclear event
products and meaure their Mössbauer specta.
Pyrite (FeS2 ) was chosen as a sample material because it has high Fe content and asimple cubic structure. A conventional cryostat for absorption Mössbauer spectroscopy
was used after slight modiﬁcation. Since scattered neutrons and the neutron beam itself
react with every material in addition to thetarget in their paths and cause unnecessary
γ-ray background. The amount of material of
the cold head holding the sample was minimized. An aluminum foil of 12 μm thickness
was used as the sample contact part of thealuminum (4N) cold head extending 20 cm
from the nitrogen vessel. This was planned tominimize the background originating from thecryostat body by placing the cryostat as far
from the beam line as possible while holding
the sample at low tempratures. The cryostat
windows were 45 mmφ holes covered with 50
μm thick Kapton foils to reduce the amount

100

106
78K
104
102
100
−4

−2

0
2
−1
Velocity / mm s

4

Figure 1: Neutron in-beam Mössbauer spectrum of
pyrite.

分野：即発γ線分析実験（その他）㻙㻌 㻟㻠㻡㻌㻙This is a blank page.

JAEA-Review 2011-050
















4.  ᡼኿ൻಽᨆ 

4. Neutron Activation Analyses㻙㻌 㻟㻠㻣㻌㻙This is a blank page.

JAEA-Review 2011-050

4-1◊✲ࢸ࣮࣐㸸୰ᛶᏊᨺᑕ໬ศᯒἲࢆ⏝࠸ࡓ⎔ቃヨᩱ୰ 129I ⃰ᗘࡢᢕᥱ⾲   㢟㸸ᮾᾏ෌ฎ⌮᪋タ࿘㎶ࡢ⏿ᅵ୰ 129I ⃰ᗘㄪᰝᮾᾏ෌ฎ⌮᪋タ࿘㎶ࡢ⏿ᅵ୰ 129I ⃰ᗘㄪᰝᅧศ ♸ྖࠊ୰㔝 ᨻᑦࠊṊ▼ ⛱᪥ᮏཎᏊຊ◊✲㛤Ⓨᶵᵓ ᰾⇞ᩱࢧ࢖ࢡࣝᕤᏛ◊✲ᡤ ᨺᑕ⥺⟶⌮㒊⎔ቃ┘どㄢ࠙ࡣࡌࡵ࡟ࠚ
ᮾᾏ෌ฎ⌮᪋タ࡛ࡣࠊ1977 ᖺࡢ࣍ࢵࢺヨ࠿ࡿࠋࡲࡓࠊ2007 ᖺᗘࡢ ᐃ⤖ᯝࢆ⾲ 1 ࡟♧ࡍࠋ⾲ 1 ࠿ࡽࠊ༡す 2km ࠾ࡼࡧ 3km ᆅⅬࡀ㦂㛤ጞ௨᮶ࠊ2007 ᖺᗘࡲ࡛࡟⣙ 1140 ࢺࣥ

12mBq㸭kg࣭஝࡜㧗ࡃࠊ1kmࠊ8km ࡢ㡰࡟పࡢ౑⏝῭⇞ᩱࡀ෌ฎ⌮ࡉࢀࡓࠋ᤼Ẽࠊ᤼Ỉ
୰ࡢ 129 I ࡣࠊࡑࡢ኱㒊ศࡀ㝖ཤࡉࢀࡓࡢࡕ

ࡃ࡞ࡗࡓࠋࡇࢀࡽࡢ⃰ᗘࡣࠊ෌ฎ⌮᪋タ࠿ࡽࡢᨺฟ㔞ཬࡧẼ㇟ほ ࢹ࣮ࢱࢆ⏝࠸ࡓᣑᩓィ⟬኱Ẽ࠾ࡼࡧᾏὒ࡬⟶⌮ᨺฟࡉࢀ࡚ࡁࡓࠋࡋ

࡟ࡼࡾࠊಖᏲⓗ࡟෌⌧ࡉࢀࡿ 2)ࠋࡲࡓ⃰ᗘⓗ࡟࠿ࡋࠊ129I ࡣ≀⌮ⓗ༙ῶᮇࡀ 1570 ୓ᖺ࡜㛗ࡃࠊᚤ㔞࡛࠶ࡗ࡚ࡶ㛗ᮇⓗ࡞ほⅬ࠿ࡽᅵተࡣࠊ㐣ཤࡢ኱Ẽᅪෆ᰾ᐇ㦂ࣇ࢛࣮ࣝ࢔࢘ࢺ࡟㉳㸦ཎᏊຊᶵᵓ࿘㎶ 2007ᅉࡍࡿ⾲ᅵ୰ 137Cs ⃰ᗘ➼ࢆᑐ㇟࡟ศᕸ࠾ࡼࡧᣲືࢆㄪᰝࡋ࡚࠸ࡿࠋ

ᖺᗘ㸸7.1㹼18Bq㸭kg࣭஝㸧࡜ẚ࡭ᩘ 100 ศࡢ࠙⏿ᅵ୰ 129I ࡢศᯒ࣭1 ௨ୗ࡛࠶ࡾࠊ⎔ቃᏳ඲ୖࠊၥ㢟ࡣ࡞࠸ࣞ࣋ࣝ
࡛࠶ࡗࡓࠋ

ᐃ᪉ἲࠚ

 ㄪᰝࡣࠊ㐣ཤࡢ඲᪉఩ࡢỈ‽ㄪᰝ⤖ᯝ࡟ᇶ࡙࢘⣲ࢆ⢭〇ࡋࠊ▼ⱥ࢔ࣥࣉࣝෆ࡟ᑒධࡋࠊཎᏊ

㻵⃰ᗘ䠄㼙㻮㼝㻛㼗㼓䞉஝䠅ศࡅࠊᑓ⏝⇞↝⿦⨨࡛⇞↝ࡋࠊ⇞↝࢞ࢫ୰ࡢࣚ
࢘⣲ࢆάᛶⅣ࡟ᤕ㞟ࡋࡓࠋ⁐፹ᢳฟἲ࡟ࡼࡾࣚ

㻝㻞㻥⏿ᅵࢆ 70Υ࡛஝⇱ᚋࠊ2mm ࣓ࢵࢩࣗࡢ⠠࡛

㻡㻜

⏿ᅵ୰

ࡁ㸯㸧ࠊ୺࡞㢼ୗ᪉ྥ࡛࠶ࡿ༡す᪉ྥࡢ⏿ᅵࢆᑐ㇟࡜ࡋࡓࠋ

⅔㸦JRR-3 ཪࡣ JRR-4㸧࡛୰ᛶᏊࢆ↷ᑕࡋࡓࠋ෌ᗘ⁐፹ᢳฟἲ࡛↷ᑕヨᩱࢆ⢭〇ࡋࠊᨺᑕ໬ࡉ

࠙⏿ᅵ୰ 129I ⃰ᗘࠚ ᅗ 1 ࡟ 1982 ᖺ࠿ࡽ 2007 ᖺ࡟࠿ࡅ࡚ࡢ༡す᪉ྥࡢ⏿ᅵ୰ 129I ⃰ᗘࡢ⤒ᖺኚ໬ࢆ♧ࡍࠋᅗ㸯ࡼࡾࠊ㢧ⴭ࡞ቑຍࡣㄆࡵࡽࢀ࡚࠸࡞࠸ࡇ࡜ࡀࢃ

㻝㻜

㻝㻥㻤㻡

㻝㻥㻥㻜

㻝㻥㻥㻡

㻞㻜㻜㻜

㻞㻜㻜㻡

ᅗ㸯 ᮾᾏ෌ฎ⌮᪋タ࿘㎶ࡢ⏿ᅵ୰ 129I ⃰ᗘࡢ⤒ᖺኚ໬
⾲ 1 ᮾᾏ෌ฎ⌮᪋タ࿘㎶ࡢ⏿ᅵ୰ 129I ⃰ᗘ㸦2007 ᖺᗘ㸧༢఩㸸mBq㸭kg࣭஝

༡す1km ༡す2km ༡す3km ༡す8km
11
12
12
2.5

ᐃࡋࠊ127I ࠾ࡼࡧ 129I ⃰ᗘࢆࡼࡾศᯒᅇ཰⋡ࢆồࡵࠊ129I ࡢ್ࢆ⿵ṇࡋࡓࠋ㻞㻜ᖺࡓࠋ᭱⤊ⓗ࡟ࠊ127I㸦n,2n㸧126Iࠊ129I㸦n,Ț㸧
130I ཯ᛂ࡟ࡼࡾ⏕ᡂࡋࡓ 126I ࠾ࡼࡧ 130I ࢆ Geᐃ㔞ࡋࡓࠋู࡟ ICP-MS ࡛ ᐃࡋࡓ 127I ⃰ᗘ࡜୰ᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡿ 127I ⃰ᗘࡢẚ⋡࡟

㻟㻜

㻜
㻝㻥㻤㻜

ࢀࡓᚤ㔞ࡢ⮯⣲➼ࢆ㝖ཤࡋࣚ࢘໬㖟ỿẊ࡜ࡋ༙ᑟయ᳨ฟჾ࡛

༡す㻝㼗㼙
༡す㻞㼗㼙
༡す㻟㼗㼙
༡す㻤㼗㼙

㻠㻜

ཧ⪃ᩥ⊩
㸯㸧Ṋ▼௚ , ⎔ቃヨᩱ୰ࡢ 127I ཬࡧ 129I ࡢ୰ᛶ Ꮚ ᨺ ᑕ ໬ ศ ᯒ ἲ , PNC TN843-85-39 ,㸦1985㸧
㸰 㸧 Nakano,M. et al, Proceeding of theInternational Symposium on Environmental
Modeling Radioecology ,㸦2006㸧, 216-222.

ཎᏊ⅔㸸JRR-3     ⿦⨨㸸Ỉຊ↷ᑕタഛ    ศ㔝㸸ᨺᑕ໬ศᯒ㸦⎔ቃ⛉Ꮫ㸧㻙㻌 㻟㻠㻥㻌㻙

JAEA-Review 2011-050

4-2⎇ⓥ࠹࡯ࡑ㧦᡼኿✢㒐⼔࡮✢㊂⹏ଔߦ㑐ߔࠆ⎇ⓥ
⴫   㗴㧦᳓㌁ਛ↢ᚑ࠻࡝࠴࠙ࡓߩᕈ⁁⸃᣿᳓㌁ਛߦᩭ෻ᔕߢ↢ᚑߐࠇࠆ࠻࡝࠴࠙ࡓߩൻቇᒻߦኻߒ᳓ಽỚᐲ߇෸߷ߔᓇ㗀⌀ㄝஜᄥ㇢‫ޔ‬ᮮጊ㗇⟤⁛┙ⴕ᡽ᴺੱᣣᧄේሶജ⎇ⓥ㐿⊒ᯏ᭴ ේሶജၮ␆Ꮏቇ⎇ⓥㇱ㐷 ᡼኿✢㒐⼔⎇ⓥࠣ࡞࡯ࡊᄢᒝᐲ㓁ሶടㅦེᣉ⸳㧔J-PARC㧕ߩ‛⾰࡮↢ሹ೨ߦ⹜ᢱߣ Co ࡈ࡜࠶ࠢࠬࡕ࠾࠲ࠍ⸳⟎ߒ‫ޔ‬๮⑼ቇታ㛎ᣉ⸳ߦ⸳⟎ߐࠇࠆਛᕈሶḮߪ‫ޔ‬ᶧ૕ᾲਛᕈሶࡕ࡯࠼Σߢ 6 ᤨ㑆ᾖ኿ߒߚ‫ޕ‬᡼኿ൻߒ㊄ዻ࠲࡯ࠥ࠶࠻ߦ 3 GeV ߩ㓁ሶࡆ࡯ࡓࠍ౉኿

ߚ Co ߩJ✢ࠬࡍࠢ࠻ࡠࡔ࠻࡝ߦࠃࠅ᳞߼ߚᾲ

ߒᩭ⎕⎈෻ᔕࠍ⿠ߎߐߖ‫ޔ‬ਛᕈሶࠍ↢ᚑߐߖࠆਛᕈሶࡈ࡜࠶ࠢࠬߪ⚂ 1.6 × 109 cm?2 s?1 ߢ޽ߞᣉ⸳ߢ޽ࠆ‫ޕ‬᳓㌁࠲࡯ࠥ࠶࠻ߪ‫ޔ‬ᩭ⎕⎈෻ᔕߦߚ‫↢ޕ‬ᚑߒߚ࠻࡝࠴࠙ࡓߪ HTO ߣ HT ߦಽ೎‫ޔ‬

ࠃࠅᄢ㊂ߦ⊒↢ߔࠆᾲࠍಣℂߔࠆߚ߼ߩᯏེ‫ޔ‬࿁෼ߒ‫ޔ‬ᶧ૕ࠪࡦ࠴࡟࡯࡚ࠪࡦࠞ࠙ࡦ࠲ߦࠃࠅ

㓁ሶࡆ࡯ࡓߩⴣ᠄ᵄߦࠃࠆౝ࿶ߩᄌൻࠍ✭ⴣ᡼኿⢻ࠍ⸘᷹ߒߚ‫ޕ‬෼₸ߪ߶߷ 100%ߢ޽ߞߚ‫ޕ‬ߔࠆࡋ࡝࠙ࡓࠟࠬࠍలႯߒߚࠨ࡯ࠫ࠲ࡦࠢ╬࿑ 1 ߦ‫⹜ޔ‬ᢱኈེ᳇⋧ߩ᳓ಽ࿶㧔Pwater㧕ߣ‫ޔ‬ࠍ஻߃ߚ࠲࡯ࠥ࠶࠻บゞౝࠍᓴⅣߔࠆ‫ޕ‬ᩭ⎕⎈↢ᚑߒߚ࠻࡝࠴࠙ࡓߩ߁ߜ HTO ߇භ߼ࠆഀว

෻ᔕߢ↢ᚑߔࠆᄙ᭽ߥ᡼኿ᕈᩭ⒳ߪ‫ࠟ࡞ࡑࠕޔ‬㧔RHTO㧕ߩ㑐ଥࠍ␜ߔ‫ޕ‬RHTO ߣ Pwater ߦߪᱜߩࡓൻߒߡ᳓㌁ߣߣ߽ߦᓴⅣ‫ߪ޿ࠆ޽ޔ‬ᴉố߹ߚ⋧㑐߇޽ࠅ‫ޔ‬࿑ 1 ߆ࠄ㑐ଥᑼࠍᓧߚ‫ޕ‬
RHTO (%) = 62 + 4.1 u ln(Pwater / Pa).

ߪ᳇ൻߒߡࠨ࡯ࠫ࠲ࡦࠢߦ⾂⬿ߐࠇࠆ‫ޕ‬᳓㌁࠲࡯ࠥ࠶࠻ਛߦ↢ᚑߔࠆ᡼኿ᕈᩭ⒳ߩ

ߔߥࠊߜ‫ߩߎޔ‬ᑼࠍ↪޿ࠇ߫‫ߦࠢࡦ࠲ࠫ࡯ࠨޔ‬߁ߜ‫ޔ‬᡼኿⢻ߩ⚂ 6 ഀߪ࠻࡝࠴࠙ࡓߢ޽ࠆ‫࠻ޕ‬ዉ౉ߔࠆࠟࠬߩ᳓ಽ࿶߆ࠄ‫ޔ‬᳓㌁࠲࡯ࠥ࠶࠻ਛ

࡝࠴࠙ࡓߪ᳇ൻߒ߿ߔ޿ߚ߼ⓨ᳇ਛߦᶋㆆߒ‫ޔ‬ߦ↢ᚑߔࠆ࠻࡝࠴࠙ࡓߩൻቇᒻߩഀว߇ផ᷹

ౝㇱⵍ߫ߊࠍᒁ߈⿠ߎߔน⢻ᕈ߇޽ࠆ‫߇ߚߒޕ‬ߢ߈ࠆ‫ߩࡓ࠙࠴࡝࠻ޔࠅࠃߦࠇߎޕ‬ൻቇᒻࠍ⠨ߞߡ‫ߦࡓ࠙࠴࡝࠻ޔ‬ኻߔࠆ✢㊂⹏ଔ߇㊀ⷐߣߥ

ᘦߒߚ✢㊂⹏ଔ߇น⢻ߦߥࠆߣ⠨߃ࠄࠇࠆ‫ޕ‬ࠆ߇‫ߩߘߪࡓ࠙࠴࡝࠻ޔ‬ൻቇᒻߦࠃࠅ៨ข㊂ᒰ
ߚࠅߩ✢㊂߇ᄢ߈ߊ⇣ߥࠆ‫࠴࡝࠻ޔ߼ߚߩߘޕ‬࠙ࡓߦࠃࠆ✢㊂ࠍ⷗Ⓧ߽ࠆߦߪൻቇᒻߦ㑐ߔࠆ⍮⷗߇ਇนᰳߢ޽ࠆ‫ޕ‬ᤓᐕᐲ߹ߢߦᚒ‫ޔߪޘ‬ᓸ㊂ߩ࡝࠴࠙ࡓࠍ฽߻
᳓㌁⹜ᢱࠍᾲਛᕈሶᾖ኿ߒ‫ޔ‬᳓㌁ࡑ࠻࡝ࠢࠬਛ
ߦࡎ࠶࠻ߥ࠻࡝࠴࠙ࡓࠍ↢ᚑߐߖ‫ࡓ࠙࠴࡝࠻ޔ‬᳓㧔HTO㧕ߣ࠻࡝࠴࠙ࡓࠟࠬ㧔HT㧕ߦಽ೎ߒ࿁෼ߔࠆᣇᴺࠍ⏕┙ߒߚ 1)‫੹ޕ‬ᐕᐲߪ‫ޔ‬᳓㌁ߦ฽߹ࠇࠆᓸ㊂ߩ᳓ಽ߇࠻࡝࠴࠙ࡓߩൻቇᒻഀ
วߦਈ߃ࠆᓇ㗀ࠍ⺞ߴߚ‫ޕ‬
᳓ಽ฽᦭㊂ࠍ⺞ᢛߒߚ᳓㌁⹜ᢱߪ‫ޔ‬ᶧ⋧ߦ௖߆ߦṁሽߔࠆ᳇૕㊂ߪ᳇⋧ߩಽ࿶ߦᲧ଀ߔࠆ
ߎߣࠍ೑↪ߒ‫ޔ‬છᗧߩ᳓ಽ࿶ߦ⺞ᢛߒߚࠟࠬࠍ

࿑ 1 ⹜ᢱኈེ᳇⋧ߩ᳓ಽ࿶ߣ↢ᚑߒߚ࠻࡝࠴࠙ࡓߩ߁ߜ HTO ߇භ߼ࠆഀวߩ㑐ଥෳ⠨ᢥ₂᳇⋧ߦዉ౉ߒ⺞ᢛߒߚ‫⹜ޕ‬ᢱߩᾲਛᕈሶᾖ኿ߪ‫ ޔ‬1) K. Manabe and S. Yokoyama, Appl. Radiat.
Isotopes 66 (2008) 122-125.
JRR-4 ߩਛᕈሶࡆ࡯ࡓ⸳஻ࠍ૶↪ߒߚ‫ࡓ࡯ࡆޕ‬૶↪ේሶἹ㧦JRR-4  ⵝ⟎ฬ㧦ਛᕈሶࡆ࡯ࡓ⸳஻  ೑↪ಽ㊁㧦᡼኿ൻಽᨆ࡮ߘߩઁ㻙㻌 㻟㻡㻜㻌㻙

JAEA-Review 2011-050

4-3
⦤≧Ⅳ㓟ሷሁ✚≀㸦ࢺࢗࣇ࢓㸧ࡢᒙูඖ⣲ศᯒ
Analysis of element in annually layered terrestrial carbonates (Tufa )஑ᕞ኱Ꮫ ࢔࢖ࢯࢺ࣮ࣉ⥲ྜࢭࣥࢱ࣮ ᮡཎ┿ྖ஑ᕞ኱Ꮫ ኱Ꮫ㝔⌮Ꮫᗓ ᳃㛗୍ᮁࠊᗈ℩⠜ᚿᅗ㸯 ࢺࢗࣇ࢓ヨᩱ↷ᑕࡣࠊ-55 Ẽ㏦⟶㸦 ⛊↷ᑕࠊ┤ᚋ࡟ ᐃ㸧ࠊ
6 ࣃ࢖ࣉ㸦 ᫬㛫↷ᑕࠊ 㐌㛫ࠊ ࣨ᭶෭༷ᚋ ᐃ㸧࡛⾜ࡗࡓࠋヨᩱ⣙ 㹫㹥ࢆ࣏࢚ࣜࢳࣞࣥ⿄ࠊ⣙ 㹫㹥ࢆ▼ⱥ⟶࡟ᑒධࡋࡑࢀࡒࢀ↷ᑕࡋࡓࠋẚ㍑ᶆ‽
ࡣ -% ࢆ฼⏝ࡋࠊ ᫬㛫↷ᑕ࡟ࡘ࠸࡚ࡣࠊ. ἲࡶ㐺ᛂࡋࡓࠋヨᩱࡣࠊ᪂ࡋ࠸㒊ศ㸦1R㸧࠿ࡽ 1R ࡲ࡛࠶ࡾࠊ
ᖺ⦤ࡢィ ࡀ☜࠿࡛࠶ࢀࡤ⣙  ᖺ࡟┦ᙜࡍࡿࠋ

㸦㸱㸧⤖ᯝ࡜⪃ᐹᰩᓮࡽ࡟ࡼࡿࠊᖺ⦤࠿ࡽᖺ௦࡙ࡅࡉࢀࡓࢺࢗࣇ࢓
ࡢ 62⃰ᗘࡢ ᐃ⤖ᯝࢆᅗ㸰࡟♧ࡍࠋ

1500

Concentration of SO42- /ppm

㸦㸯㸧 ࡣࡌࡵ࡟
⦤≧Ⅳ㓟ሷሁ✚≀㸦ࢺࢗࣇ࢓㸧ࡣࠊ㝣ᇦ࡛⏕ᡂࡍ
ࡿⅣ㓟ሷሁ✚≀࡛࠶ࡾࠊ▼⅊ᒾᆅᇦࡢ‪ἨࡸἙᕝࠊ
†ࡢ⁄ὶ㒊࡟ሐࡸ⁪ࢆᙧᡂࡍࡿࠋከᏍ㉁࡛ࠊ⸴㢮࣭᳜≀᰿࡞࡝ࡢ⑞㊧ࢆࡶࡕࠊ⣽⢏㉁ࡢⅣ㓟࢝ࣝࢩ࣒࢘
ࡀࡺࡿࡃᅛ⤖ࡋࡓሁ✚≀࡛࠶ࡿࠋỈࡢ⵨Ⓨࠊ⬺஧㓟໬Ⅳ⣲࡟ࡼࡾⅣ㓟࢝ࣝࢩ࣒࡛࢘㐣㣬࿴࡟࡞ࡗࡓỈ࠿ࡽࠊࢩ࢔ࣀࣂࢡࢸࣜ࢔㸦⸛⸴㢮㸧ࠊ⥳⸴㢮ࠊ⹊ⱏ㢮࡟ࡼࡿගྜᡂ࡟ࡼࡾࡉࡽ࡟⁐Ꮡ஧㓟໬Ⅳ⣲ࡀᾘ㈝ࡉࢀ
࡚㐣㣬࿴ࡀ㐍⾜ࡋࠊⅣ㓟࢝ࣝࢩ࣒࢘ࡀỿẊࡍࡿ࡜⪃࠼ࡽࢀ࡚࠸ࡿࠋࡑࡢࡓࡵࢺࢗࣇ࢓ࡣࠊᖺ㍯ࡢࡼ࠺࡟
⦤≧࡟Ⓨ㐩ࡍࡿࠋ⦤࡟ࡣሁ✚ᙜ᫬ࡢ⎔ቃࢆಖᣢࡋ࡚
࠸ࡿࠋࡇࡢࡓࡵࠊ⦤ࡢᩘࢆィ ࡍࡿࡇ࡜࡟ࡼࡾࠊ⤯ᑐᖺ௦ࡀ᥎ᐃྍ⬟࡛࠶ࡾࠊࡑࡢ⦤࡟ྵ᭷ࡍࡿඖ⣲ศᕸࢆ ᐃࡍࢀࡤࠊࡑࡢᙜ᫬ࡢ⎔ቃởᰁ≀㉁➼ࡢ㝆ୗࡢᙳ㡪ࢆ▱ࡿࡇ࡜ࡀ࡛ࡁࡿࠋ௒ᅇࠊ⚟ᒸ┴ࡢ▼⅊ᒾᆅ༊࡛࠶ࡿᖹᑿྎ࡛᥇ྲྀࡋࡓࢺࢗࣇ࢓࡟ࡘ࠸࡚ࠊ୰
ᛶᏊᨺᑕ໬ศᯒࢆ㐺ᛂࡋࠊඖ⣲ศᕸࢆ ᐃࡋࠊ໭஑
ᕞᆅ༊࡟࠾ࡅࡿ⎔ቃởᰁࡢṔྐࢆゎ᫂ࡍࡿࠋ
ᰩᓮࡽࡣࠊྠヨᩱࢆ⏝࠸࡚ࠊ⾲ὶỈ࡜ࡢ࢖࢜ࣥ஺
᥮཯ᛂ࡟ࡼࡗ࡚ಖᣢࡋ࡚࠸ࡿ኱Ẽởᰁࡢᣦᶆ࡜࡞ࡿ
62⃰ᗘࡢ ᐃ࠿ࡽࠊ໭஑ᕞᆅ༊࡟࠾ࡅࡿ㐣ཤࡢ኱Ẽởᰁࡢኚ㑄ࡢ᚟ඖࢆ⾜࠺ࡇ࡜ࡀ࡛ࡁࡓࠋ௒ᅇࡣࠊ
኱Ẽởᰁ≀㉁➼ࡢ⎔ቃ᝟ሗࢆᢳฟࡍࡿࡓࡵ࡟ࠊྛඖ
⣲⃰ᗘࢆ ᐃࡋࡓࠋ
㸦㸰㸧ᐇ㦂࡜᪉ἲ
ヨᩱࡣࠊ⚟ᒸ┴ࡢᖹᑿྎ࡛᥇ྲྀࡋࡓࠋ஝⇱ᚋࠊᒙู࡟ศูࡋศᯒ⏝ヨᩱ࡜ࡋࡓࠋ

1300
1100
900
700
500
300
1943

1953

1963

1973

1983

1993

Age /yrᅗ㸰 ࢺࢗࣇ࢓୰ࡢ SO42-⃰ᗘᖺኚ໬ ᖹᑿྎࡣࠊ໭஑ᕞᕷࡢ༡᪉⣙ 20km ࡟࠶ࡿࠋ໭
஑ᕞᕷࡣࠊ1946 ᖺࡢඵᖭ〇㕲✌ື࡟ࡼࡾᛴ㏿࡟ᕤᴗ໬ࡉࢀ⎔ቃởᰁࡀⓎ⏕ࡋ࡚࠸ࡿࠋᅗ㸰࠿ࡽࢺࢗࣇ࢓୰ࡢ◲㓟࢖࢜ࣥ⃰ᗘࡶྠ᫬ᮇ࠿ࡽᛴ⃭࡟ୖ᪼ࡋ࡚࠸ࡿࡀࠊ60 ᖺ௦࠿ࡽࡣ࡯ࡰᆒ୍ࡢ⃰ᗘࢆࡋ
ࡵࡋࠊ90 ᖺ௦࡛ࡣపୗࡋ࡚࠸ࡿࠋࢺࢗࣇ࢓⾲㠃ࡢ㒊ศ㸦⣙ 10 ᖺศ㸧ࡣࠊእほୖࡶ␗࡞ࡗ࡚࠸ࡿࠋ
ࡋ࠿ࡋࠊ◲㓟࢖࢜ࣥ⃰ᗘ࠿ࡽ኱Ẽởᰁࡢᙳ㡪ࡣࡇࡢࡼ࠺࡟ࢺࢗࣇ࢓୰࡟ほ ࡍࡿࡇ࡜ࡀ࡛ࡁࡓࠋ ௒ᅇࠊᨺᑕ໬ศᯒ࡛ ᐃࡋࡓඖ⣲ࡣࠊAl, Ca, Ce,
Co, Cr, Eu, Fe, Hf, La, Mn, Sc, Sm, Th, Ti, V, Lu, Mg,
Na, Se, Yb, Ba, Cs, Ta, U ࡛࠶ࡿࠋ඲࡚ࡢඖ⣲ࡀࠊྛヨᩱ࡟᳨ฟࡉࢀࡓࢃࡅ࡛ࡣ࡞࠸ࡢ࡛ࠊ50㸣௨ୖࡢヨᩱ᳨࡛ฟࡉࢀࡓࠊ15 ඖ⣲࡟ࡘ࠸࡚ࠊኚືࢆࡳࡓࠋ

JRR-4 Ẽ㏦⟶ S ࣃ࢖ࣉ ⎔ቃヨᩱᨺᑕ໬ศᯒ㻙㻌 㻟㻡㻝㻌㻙

JAEA-Review 2011-050

 ࡲࡎࠊCa ࡢศᕸ࡛࠶ࡿࡀࠊࢺࢗࣇ࢓ࡢ୺ᡂศ࡛࠶
ࡿⅣ㓟 Ca ࡢ⃰ᗘࡣࠊᖹᆒࡋ࡚ 96%࡛࠶ࡾࠊCa ⃰ᗘࡣ⣙ 3.8105 ppm ࡜࡞ࡿࠋ5.E+05Ca [ppm]

4.E+05

᥇ྲྀᆅⅬࡣࠊ㏻ᖖேࡀฟධࡾࡍࡿᡤ࡛ࡣ࡞࠸ࡢ
࡛ࠊ኱Ẽ࠿ࡽࡢ㝆ୗ㔞ࡢኚື࠿ࠊ࿘㎶ࡢ㛤Ⓨ㸦᳜ᯘ➼㸧࡟ࡼࡿᑠἙᕝ࡬ࡢὶධࡢኚືᙳ㡪࠿ࡀ⪃࠼ࡽࢀࡿࠋ ḟ࡟⃰ᗘࡢኚືࡀ࠶ࡲࡾ࡞࠸ඖ⣲ࡣࠊMg, Na,
Eu, Hf ࡛࠶ࡾࠊ๓ 2 ඖ⣲ࡢ⃰ᗘኚ໬ࢆᅗ㸳࡟♧ࡍࠋ

3.E+058.0E+03Mg

2.E+05ppm

0.E+00
0

10

20

30

40

50

60

70

4.0E+0380 ᅗ㸱 ࢺࢗࣇ࢓୰ࡢ Ca ⃰ᗘࡢศᕸ

2.0E+03

 Ca ⃰ᗘࡣࠊ◲㓟࢖࢜ࣥ⃰ᗘࡢኚ໬࡜ẚ࡭࡚ࠊ኱ࡁ
࡞ኚ໬ࡣ࡞ࡃࠊࢺࢗࣇ࢓⮬యࡢ⏕ᡂ᮲௳࡟኱ࡁ࡞ኚ
ືࡣ࡞࠿ࡗࡓࡇ࡜ࡀࢃ࠿ࡿࠋ ࡑࡢ௚ࡢඖ⣲࡛ࡣࠊ⾲㠃࠿ࡽ 10㹼12 ␒┠࡟࠿ࡅ࡚኱ࡁ࡞ኚືࡀぢࡽࢀࡿඖ⣲࡜ࠊぢࡽࢀ࡞࠸ඖ⣲࡟኱ࡁࡃ኱ู࡛ࡁࡓࠋኚືࡀぢࡽࢀࡿඖ⣲ࡢ౛࡜ࡋ࡚ࠊ
Al ࡜ Fe ࡢ⃰ᗘศᕸࢆᅗ 4 ࡟♧ࡍࠋ

0.0E+00Al
2.0E+04Feppm

1.5E+04
1.0E+04
5.0E+03
0.0E+00
10

20

30

40

50

60

70

80

 ᅗ㸲 ࢺࢗࣇ࢓୰ࡢ AlࠊFe ⃰ᗘศᕸ ⾲ᒙ 10 ␒┠ࡲ࡛⃰ᗘࡀቑຍࡋࠊࡑࡢᚋᛴ⃭࡟ῶᑡࡋ࡚ࡑࡢᚋ 70 ␒┠ࡲ࡛ࡣ࡯ࡰᆒ୍ࠊ᭦࡟ࡑ
ࡢᚋୖ᪼ࡍࡿࠋྠᵝࡢኚືࢆ♧ࡍඖ⣲ࡣࠊCe, Co,
Cr, La, Mn, Sc, Sm, Th, Ti, V, Lu ࡛࠶ࡗࡓࠋ⾲ᒙࡢኚ໬ࡣ◲㓟࢖࢜ࣥ⃰ᗘ࡛ࡶྠᵝࡢኚ໬ࢆ♧ࡋࠊእほୖࡶ⾲㠃ࡣⱝᖸⰍࡀ␗࡞ࡿࡓࡵࠊẚ㍑ⓗ᪂ࡋ࠸㸦10 ᖺ⛬ᗘ㸧㒊ศࡣࢺࢗࣇ࢓࡟ྲྀࡾ㎸ࡲࢀࡿ⢓ᅵ㖔≀➼ࡢ⤌ᡂࡀ␗࡞ࡾఱࡽ࠿ࡢ⎔ቃኚືࡀ㉳ࡇࡗࡓࡇ࡜ࡀ⪃࠼ࡽࢀࡿࠋࡋ࠿ࡋࠊࡇࡢᖺ௦࡟┦ᙜࡍࡿᖹᑿྎ࡟࠾ࡅࡿ࢖࣋ࣥࢺ࡟ࡘ࠸࡚ࡣࡣࡗࡁ
ࡾࡋ࡞࠸ࠋ᭦࡞ࡿ᳨⣴ࡀᚲせ࡛࠶ࡿࠋྂ࠸㒊ศࡢ⃰ᗘୖ᪼࡟ࡘ࠸࡚ࡶࠊཎᅉࡣࡲࡔࢃ࠿ࡽ࡞࠸ࠋ

0

10

20

30

40

50

60

70

80

  ᅗ㸳 ࢺࢗࣇ࢓୰ࡢ Mg, Na ⃰ᗘศᕸ ᅗ 4 ࡟ぢࡽࢀࡓࡼ࠺࡞ኚືࡣ࡞࠸ࠋ ᐃ㔞ࡋࡓඖ⣲㸦Ca ࢆ㝖ࡃ㸧ࡢᖹᆒ⃰ᗘࢆィ⟬ࡍࡿ࡜ࠊከ࠸᪉࠿ࡽ Al(1.2%), Mg(0.4%),Na(0.06%),
Fe(0.05%)࡜࡞ࡾṧࡾࡣࠊᩘ༑ ppm ࡛࠶ࡿࠋࡇࢀ
ࡽࡢ 4 ඖ⣲࡛ኚືࡀ␗࡞ࡿࡇ࡜࠿ࡽࠊ2 ✀㢮ࡢ⢓ᅵ㖔≀ࡢ⤌ᡂࡀ␗࡞ࡗࡓࡢ࡛ࡣ࡞࠸࠿࡜⪃࠼ࢀࡿࠋ ࡉࡽ࡟ࠊ኱Ẽởᰁ≀㉁➼ࡢ⎔ቃ᝟ሗᢳฟ࡟ࡘ࠸࡚
ࡣࠊ࿘㎶ࡢ⎔ቃኚື࡜ࡢ㑅ูࢆ⾜࠺ᚲせࡀ࠶ࡿࡓࡵ⌧≧࡛ࡣ᩿ᐃ࡛ࡁ࡞࠸ࠋ
 ࿘㎶ᅵተࡢᙳ㡪ࢆホ౯ࡍࡿࡓࡵ࡟ࠊࢺࢗࣇ࢓⏕ᡂሙᡤࡢୖὶᆅⅬ࡛ࠊᅵተࢥ࢔ࢆ 2 ᮏ᥇ྲྀࡋࠊ2cm
ࡈ࡜࡟ษ᩿ࡋ஝⇱ᚋࠊGe ༙ᑟయ᳨ฟჾ࡛࣐࢞ࣥ⥺ࢆ ᐃࡋࡓࠋ⾲㠃ᅵተࢥ࢔࡟࠾ࡅࡿ 137Cs ࡜ 210Pb
ࡢ῝ᗘศᕸࢆᅗ㸴ࠊ㸵࡟♧ࡍࠋ
4.5E-02
core1
core2
Cs-137 [Bq/ g dry soil]

2.5E+040Na

6.0E+03

1.E+05

3.0E-02

1.5E-02

0.0E+00
1

2

3

4

5

6

7

8

9 10 11 12 13 14 15 16 ᅗ㸴 ᅵተࢥ࢔୰ࡢ 137Cs ῝ᗘศᕸࢥ࢔㸯࡛ࡣࠊ⾲ᒙࡀᑡࡋᾐ㣗࣭᧠஘ࡉࢀ࡚࠸ࡿ

4-3

㻙㻌 㻟㻡㻞㻌㻙

JAEA-Review 2011-050

ࡀࠊࢥ࢔㸰࡛ࡣࠊ60 ᖺ௦๓༙࡜ᛮࢃࢀࡿ 137Cs ࡢࣆ࣮ࢡࡀṧࡗ࡚࠸ࡿࠋࡇࡢࡼ࠺࡟᫂ࡽ࠿࡟ୖᒙ⣙20cm ࡟኱Ẽ㝆ୗ≀⏤᮶ᨺᑕᛶ᰾✀ࡢ⵳✚ࡀぢࡽࢀࡿࡢ࡛ࠊࢺࢗࣇ࢓⏕ᡂ᫬࡟ࡇࢀࡽࡢ኱Ẽ㝆ୗ≀ࡀྲྀࡾ㎸ࡲࢀಖᏑࡉࢀ࡚࠸ࡿࡇ࡜ࡀ☜ㄆ࡛ࡁࡓࠋ
8.0E-03

Pb-210 [Bq/ g dry soil]

core1
core2
6.0E-03

4.0E-032.0E-03

0.0E+00
1

2

3

4

5

6

7

8

9 10 11 12 13 14 15 16ᅗ㸵 ᅵተࢥ࢔୰ࡢ 210Pb ῝ᗘศᕸPb ῝ᗘศᕸ࡟࠾࠸࡚ࡶࠊ⣙ 20cm ࡲ࡛ᚎࠎ࡟
ῶᑡࡋᾐ㣗࣭᧠஘ࡢ኱ࡁ࡞ኚ໬ࡣほ ࡉࢀ࡞࠸ࠋ
210௒ᅇ᥇ྲྀࡋࡓࠊࢺࢗࣇ࢓ヨᩱ࡟ࡘ࠸࡚ࠊᨺᑕ໬
ศᯒ࡟ࡼࡗ࡚ඖ⣲ศᯒࢆ⾜ࡗࡓࠋ◲㓟࢖࢜ࣥ⃰ᗘ࡟ほ ࡉࢀࡓࡼ࠺࡞ኚືࢆほ ࡍࡿࡇ࡜ࡀ࡛ࡁ
ࡓࡀࠊࡑࡢཎᅉ࡟ࡘ࠸࡚ࡣࠊ኱Ẽởᰁࡢᙳ㡪࡞ࡢ࠿࿘㎶⎔ቃࡢኚື࡞ࡢ࠿ࢆࠊ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࡣ
ฟ᮶࡞࠿ࡗࡓࠋࡋ࠿ࡋࠊඖ⣲⃰ᗘࡢศᕸࣃࢱ࣮ࣥ
ࡀ␗࡞ࡿඖ⣲ࡀᏑᅾࡋࠊࢺࢗࣇ࢓ࡢ⏕ᡂ⎔ቃࡢኚ໬ࡀぢࡽࢀࡿࡇ࡜ࡀࢃ࠿ࡾࠊࡑࡢཎᅉ࡟ࡘ࠸࡚᭦
࡞ࡿㄪᰝࡀᚲせ࡛࠶ࡿࠋ኱Ẽởᰁࡔࡅ࡛࡞ࡃࠊ࿘㎶⎔ቃࡢኚືࢆ᥎ᐹࡍ
ࡿᡭẁ࡜ࡋ࡚ࡣࠊከඖ⣲ࢆศᯒࡋ⥲ྜⓗ࡟ุ᩿ࡍࡿᡭἲࡣ᭷ព⩏࡛࠶ࡾࠊᖹᑿྎࡢ㛤ⓎࡢṔྐ➼࡜↷ྜࡋ࡚ࠊኚືࡢཎᅉࢆ᥈ࡿࡇ࡜ࡀྍ⬟࡛࠶ࡿࠋ㸦㸲㸧ཧ⪃ᩥ⊩ᰩ ᓮ ᘯ ㍜ 㸸 ([WUDFWLRQ RI HQYLURQPHQWDOLQIRUPDWLRQ IURP DQQXDOO\ OD\HUHG WHUUHVWULDOFDUERQDWHVᖹᡂ  ᖺᗘ஑ᕞ኱Ꮫ኱Ꮫ㝔⌮Ꮫᗓಟ
ኈㄽᩥ




4-3

㻙㻌 㻟㻡㻟㻌㻙

JAEA-Review 2011-050

4-4

ࠕᕤሙ㊧ᆅ࡟࠾ࡅࡿᅵተởᰁ᳜≀ί໬ἲࡢ᳨ウࠖ
6WXGLHVRQ3K\WRUHPHGLDWLRQ RI6RLO3ROOXWLRQVDWWKHWUDFHRIDIDFWRU\ᕝすᖾᏊ(Ṋⶶ㔝Ꮫ㝔኱Ꮫ)ࠊ㔝ᕝ᠇ኵࠊᕳฟ⩏⣫(ᮾி኱Ꮫ࢔࢖ࢯࢺ࣮ࣉ⥲ྜࢭࣥࢱ࣮)
 ⃝ᖭᾈஅࠊᕝᡭ⛱ࠊ▼ᮏග᠇(ᮾி኱Ꮫ኱Ꮫ㝔ᕤᏛ⣔◊✲⛉ཎᏊຊᑓᨷඹྠ฼⏝⟶⌮ᮏ㒊)ᯇỤ⚽᫂㸦ཎᏊຊᶵᵓཎᏊຊ⛉Ꮫ◊✲ᡤ㔞Ꮚࣅ࣮࣒ᛂ⏝◊✲㒊㛛୰ᛶᏊ⏘ᴗ฼⏝ᢏ⾡◊✲ࣘࢽࢵࢺ㸧
ᕷ㈍ᅬⱁ⏝ᅵᡈࡣởᰁᅵተ࡟ヨ⸆⁐ᾮ,Sb,ZnCd

㸯㸬◊✲ࡢ┠ⓗ࡜ព⩏   ௒ࠊ඲ᅜ࡛ᅵተởᰁࡢሗ࿌ࡀ┦ḟࡂࠊࡑࡢ㸴๭ࡀ⎔㸦ணࡵ NaOH,HCl ࡛୰࿴ࡋࡓ⁐ᾮ㸧ࢆຍ࠼ࡓᚋࠊ

ቃᇶ‽ࢆ㉺࠼࡚࠸ࡿࠋởᰁᑐ⟇࡟ࡣ 2 ἲᚊࠊ㎰ᆅ࡟᭦࡟Ỉࢆ඘ศ࡟ຍ࠼࡚Ỉᒙࢆಖࡘ≧ែ࡛⏕⫱ࡉࡏࡓࠋᑐࡋ࡚ࡢ㎰⏝ᆅᅵተởᰁ㜵Ṇἲࠊᕷ⾤ᆅࢆᑐ㇟࡟ࡋ

2.4㸬᱂ᇵᚋࡢศᯒヨᩱㄪ〇ࡓᅵተởᰁᑐ⟇ἲࡀ࠶ࡿࠋࡋ࠿ࡋࠊᨺ⨨໬ࠊ㝖ཤࡋ ᱂ᇵᚋࡢ᳜≀ࡣỈὙᚋࠊ᭦࡟⢭〇Ỉࢆධࢀࡓࣅ࣮

ࡓởᰁᅵࡢ⾜᪉࡞࡝㔜せ࡞ၥ㢟Ⅼࡀୖࡀࡗ࡚࠸ࡿࠋ

࣮࢝࡟ධࢀ㉸㡢ἼὙίᶵ࡛Ὑίࡋࠊ࣮࣌ࣃ࣮ࢱ࢜ࣝ

ᅵተ࡟໬Ꮫヨ⸆࡞࡝ࢆຍ࠼ࡎ࡟ࠊởᰁඖ⣲ࢆࣜࢧ࢖࡟ᅵࡀࡘ࠿࡞ࡃ࡞ࡿࡲ࡛ࠊఱᅇ࠿Ὑίࢆ⧞ࡾ㏉ࡋࠊࢡ࡛ࣝࡁࡿᙧ࡛ᅇ཰ࡍࡿ᪉ᘧ࡜ࡋ࡚᳜≀࡟ࡼࡿᢳฟ

࣮࣌ࣃ࣮ࢱ࢜ࣝ࡟ࡃࡿࡳࠊ60Υࡢ஝⇱ᶵ࡛஝⇱ࡋࡓࠋἲࢆ᳨ウࡋ࡚ࡁࡓࠋ

஝⇱᳜≀ࢆᆅୖ㒊࡜ᆅୗ㒊࡟ศࡅࠊ୍㒊ᆅୗ㒊ࡢሢ㸰㸬ᐇ㦂ᴫせ᰿(㯏㛛෤)ࢆศ㞳ࡋࠊࢭ࣑ࣛࢵࢡ〇ᑠᆺ⢊○ᶵ࡟࠿ ᕤሙ㊧ᆅ࡟㞄᥋ࡍࡿᅵተࢆධᡭࡋࠊࡑࡢᆒ୍໬ࡋ

ࡅ⢊ᮎ໬ࡋࡓࠋ

ࡓヨᩱ࡟ࡘ࠸࡚ࠊ࢔ࣥࢳࣔࣥࠊள㖄ࠊ㕲ࠊ࢝ࢻ࣑࢘

2.5㸬୰ᛶᏊᨺᑕ໬ศᯒ᮲௳

࣒ởᰁ㔞ࢆᶵჾ୰ᛶᏊᨺᑕ໬ศᯒ㸦INAA㸧࠾ࡼࡧྛヨᩱࡣཌࡉ 0.05mm ࣏ࣜ⿄࡟ධࢀ࡚ࢩ࣮ࣝࡋࠊᮾ

༶ⓎȚ⥺ศᯒ㸦PGA)࡟ࡼࡾᐃ㔞ࡋࡓࠋࡇࢀࡽࡢඖ⣲ὒࢁ⣬ 51A ࢆᣳࡳࠊࡉࡽ࡟ྠ࣏ࣜ⿄࡟ධࢀ࡚ࢩ࣮ࣝ

ࢆຠ⋡ࡼࡃ྾཰ࡍࡿ᳜≀ࢆ᳨ウࡋࡓࠋඛࡎỈ⪔᱂ᇵࡋࠊINAA ศᯒヨᩱ࡜ࡋࡓࠋ

࡛ 2 ✀ࡢ᳜≀,ࢭ࢖ࣚ࢘࢟ࢬࢱ Hedera helix Linn.

INAA ࡣ᪥ᮏཎᏊຊ◊✲ᡤᮾᾏ◊✲ᡤ㹈㹐㹐㸫㸱ཎ(࢘ࢥࢠ⛉)࠾ࡼࡧࢪࣕࣀࣄࢤ Ophiopogon japonicus

Ꮚ⅔ࠊ↷ᑕᏍ㸸㹎N㸫1㸤2㸪↷ᑕ఩⨨㸸ୗẁࠊ5.2&

Ker-Gawl.(ࣘࣜ⛉)ࡀ✀ࠎࡢ᳜≀ࢆ᳨ウࡋࡓ⤖ᯝ࠿

4.71017㸭cm2࣭sec, 20 ศ㛫↷ᑕࠊࡲࡓࠊ㹈㹐㹐ࡽ㑅ࡤࢀࡓࠋḟ࡟୧⪅ࡢ᳜≀ࡢᅵተ᱂ᇵ࡟ࡼࡿ྾཰ຊࢆ᳨ウࡋࡓࠋ

㸫㸲ཎᏊ⅔ࠊ⡆᫆↷ᑕ⟄㹒ࣃ࢖ࣉࠊ5.3&4.31017
㸭cm2࣭sec, 20 ศ㛫↷ᑕ,10 ᪥ᚋࡼࡾ ᐃࢆ㛤ጞࡋࡓࠋ

2.1.ᕤሙ㊧ᆅ㏆ഐᅵተ࠾ࡼࡧணഛᐇ㦂ᅵተ
ᕤሙ㊧ᆅࡢᩜᆅቃ⏺࠿ࡽ㸶㹫㐨㊰ࢆ㝸࡚ࡓእ㒊ࡢᐃࡣᮾி኱Ꮫ࢔࢖ࢯࢺ࣮ࣉ⥲ྜࢭࣥࢱ࣮࡛ࠊ

MODEL SC100L ᨺᑕ⬟ ᐃ⏝㐽ⶸయ௜࣮࢜ࢺࢧࣥ
ࣉࣝࢳ࢙ࣥࢪ࣮ࣕ(ᮾὒ࣓ࢹ࢕ࢵࢡ)ࢆ⏝࠸࡚,ᅵᆅ࡛ࠊ῝ࡉ㸮㸫1m ๓ᚋ᥀ࡾ㏉ࡋࡓᅵተࢆධᡭࡋࠊ

10,000sec ࡛▼ࠊ⎰♟➼ࢆ㝖ࡁࠊ஝⇱⢊ᮎ໬ࡋởᰁᶆ‽ᅵተヨᩱࢆ 13mmȭࡢ࣌ࣞࢵࢺ࡟ࡋࠊFEP ࣇ࢕࣒ࣝ࡟ᑒධࡋ

࡜ࡋࡓࠋ᳜≀ࡢࢫࢡ࣮ࣜࢽࣥࢢ࡟ࡣᕷ㈍ᅬⱁᅵተࢆ

࡚ࠊࢸࣇࣟࣥࣇ࣮࣒ࣞ࡟ྞࡾୗࡆ࡚ࠊPGA ↷ᑕ⿦⨨⏝࠸ࠊởᰁඖ⣲ࢆῧຍࡋ࡚ᐇ㦂ࡋࡓࠋ࡟タ⨨ࡍࡿࠋJRR࣮3M ༶ⓎȚ⥺ศᯒ⿦⨨(㹒㸯̿4ᐃࡋࡓࠋ PGA ࡣ⢊ᮎヨᩱ⣙ 400mg

̿1)࡛୰ᛶᏊࣅ࣮࣒㸸෭୰ᛶᏊࠊ ᐃ᫬㛫 2000 ⛊ࠊ

2.2㸬Ỉ⪔᱂ᇵᐇ㦂࢟ࢬࢱ࡞࡝✀ࠎࡢ᳜≀ࡢᗂⱑࢆ࣏ࢵࢺ࡛ධᡭࡋࠊ᰿
ࢆฟ᮶ࡿࡔࡅയࡘࡅ࡞࠸ࡼ࠺࡟Ỉ୰࡛ᰴࡈ࡜࡟ศ㞳Cd ࡣ 558KeV ࡢࣆ࣮ࢡ㠃✚ࢆᶆ‽≀㉁࡜ẚ㍑ᐃ㔞ࡋࡓࠋࡋὙίࡋࡓࠋྛῧຍඖ⣲Ỉ⁐ᾮࡣ NaOH,HCl ࡛୰࿴ᚋࠊ᳜≀ࢆධࢀࠊᡞእ࡛Ỉ⪔᱂ᇵࢆ࠾ࡇ࡞ࡗࡓࠋ
2.3.

ᅵተ᱂ᇵᐇ㦂◊✲᪋タ࡜⿦⨨ྡ㸸JRR-3,JRR-4 ࡢ INAA, JRR࣮3M ༶ⓎȚ⥺ศᯒ⿦⨨(T1̿4̿1)  ◊✲ศ㔝㸸⎔ቃ⛉Ꮫ .

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JAEA-Review 2011-050

㸱㸬⤖ᯝ࡜⪃ᐹ ᐇ㦂⤖ᯝࢆ⾲㸯࡟ࡲ࡜ࡵࡿࠋ

⾲㸯୰ᛶᏊᨺᑕ໬ศᯒཬࡧ༶ⓎȚ⥺ศᯒ㸦࢝ࢻ࣑࣒࢘ࡢࡳ㸧࡟ࡼࡿ ᐃ್㹙┦஌ᖹᆒ್㹛ởᰁᅵተࡢศᯒ್

ࠉ࢔ࣥࢳࣔࣥ

ࠉࠉள㖄⃰ᗘ㸦SSP㸧 ศ㓄ẚ㸦㸣㸧 ⃰ᗘ㸦SSP㸧





ࠉࠉࠉᕤሙ௜㏆ởᰁᅵ
ྠୖ+&Oᢳฟ㒊ྠୖᢳฟṧ㒊

Ỉ
⪔
᱂
ᇵ
ᅵ
ተ
᱂
ᇵ




ࠉ࢝ࢻ࣑࣒࢘

ศ㓄ẚ㸦㸣㸧 ⃰ᗘ㸦SSP㸧








ศ㓄ẚ㸦㸣㸧

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⃰ᗘ㸦SSP㸧 ศ㓄ẚ㸦㸣㸧 ⃰ᗘ㸦SSP㸧 ศ㓄ẚ㸦㸣㸧 ⃰ᗘ㸦SSP㸧 ศ㓄ẚ㸦㸣㸧
᳜≀✀
᱂ᇵ᮲௳
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PDJQHW྾╔㒊
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
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ᅵṧ㒊+&O㒊ࠉࠉ㸨ᅵṧ㒊

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ᅵṧ㒊+&Oṧ㒊


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ᕤሙ௜㏆ᅵተࡣ INAA ࡟ࡼࡾࠊ࢔ࣥࢳࣔࣥ

ࡓࠋࢪࣕࣀࣄࢤࡢ࢔ࣥࢳࣔࣥ྾཰ࡣሷ㓟࡟ࡼࡿᢳฟ

㸦50ppm㸧ࠊள㖄㸦1,000ppm㸧ࠊPGA ࡟ࡼࡾ࢝ࢻ࣑

16㸣࡟ẚ㍑ࡋࠊ୍ᛂ࢔ࣥࢳࣔࣥࡢί໬ἲ࡜ࡋ࡚౑⏝࣒࢘㸦15.5ppm㸧ࡢởᰁࢆ☜ㄆࡋࡓࠋ㏻ᖖࠊᅵተ୰

࡛ࡁࡿ࡜ᛮࢃࢀࡿࠋࡋ࠿ࡋࠊࢪࣕࣀࣄࢤ᱂ᇵᚋࡢᅵ

ࡢ࢔ࣥࢳࣔࣥᐃ㔞್ࡣ㸯N ሷ㓟ᢳฟ࡟ࡼࡿศᯒ್࡛

ተࢆ㸯N ሷ㓟ᢳฟࡍࡿ࡜ṧ㒊ࡢ࢔ࣥࢳࣔࣥ 3 ๭ࠊள࠶ࡿࠋᚑࡗ࡚ࠊ1N ሷ㓟࡛ᢳฟࡍࡿ࡜ࠊ࢔ࣥࢳࣔࣥ

㖄 9 ๭ࡀᢳฟࡉࢀࡓࠋ

ࡣ 21ppm 16㸣㸦ṧ㒊ࢆྵࡵࡓྵ㔞ࢆ 100 ࡜ࡋ࡚㸧ࠊள㖄ࡣ 3,000ppm ࠊ83㸣㸦ྠᕥ㸧࡜࡞ࡗࡓࠋ

ࡲࡓࠊởᰁᅵተࢆ࣐ࢢࢿࢵࢺ࡛ฎ⌮ࡋࠊ྾╔㒊ཬࡧὙᾮ㒊ࢆ㞟ࡵࠊINAA ࡛ᐃ㔞ࡍࡿ࡜ࠊ࢔ࣥࢳࣔࣥ

ࡇࢀࡽࡢ᳜≀࡛Ỉ⪔᱂ᇵࡢ⤖ᯝࡣ࢔ࣥࢳ࡛ࣔࣥࠊ

15㸣ࠊள㖄 13㸣ᅇ཰࡛ࡁࡿࠋࡑࡢᅵተ࡛᳜≀ࢆ᱂ᇵࢭ࢖ࣚ࢘࢟ࢬࢱ᰿㒊 490ppm ཰㔞 30㸣ࠊࢪࣕࣀࣄ

ࡍࡿ࡜ࠊண᝿㏻ࡾ᳜≀ࡢ྾཰㔞ࡣ࢔ࣥࢳࣔࣥࠊள㖄ࢤ᰿㒊 430ppm ᳜≀඲య࡛㸳๭ᅇ཰ࠊள㖄ࡢሙྜ࡛ඹ 2㹼5㸣࡜పࡃ࡞ࡗࡓࠋ

ࡣ᳜≀඲య࡛ࠊࢭ࢖ࣚ࢘࢟ࢬࢱ㸲๭ࠊࢪࣕࣀࣄࢤ࡛

ࡇࢀࡽࡢ⤖ᯝࡣᅵተ୰࡟࠾ࡅࡿ㕲࡜࢔ࣥࢳࣔࣥࠊ

㸶๭ᅇ཰ࡉࢀࡿ࡜ࡢ⤖ᯝࡀᚓࡽࢀࡓࠋᅉࡳ࡟ࢪࣕࣀ

ள㖄ࡢ㘒໬ྜ≀ࡢᣲື࡜⪃࠼ࡽࢀࡿࠋᅵተ୰࡟㕲⢊ࣄࢤࡢሢ᰿㒊ࡣ⏕⸆㯏㛛෤࡜ࡋ࡚౑⏝ࡉࢀࡿࡀࠊࡇ

ࢆᧈࡁࠊ࣐ࢢࢿࢵࢺ࡛ᅇ཰ࡍࡿ᪉ἲࡀ᭷ᶵሷ⣲໬ྜࡢ㒊ศࡢ࢔ࣥࢳࣔࣥࠊள㖄ࡢ྾཰㔞ࡣ 8%࡛ప࠸ࡇ≀ࡢศゎί໬ 1㸧࡜ඹ࡟ởᰁඖ⣲ࡢ㝖ཤ࡟᭷ຠ࡛࠶ࡿ

࡜ࡀࢃ࠿ࡗࡓࠋ

ࡇ࡜ࡀ♧၀ࡉࢀࡓࠋ

ࡇࢀࡽࡢ᳜≀࡛ᅵተ᱂ᇵࡋࠊ྾཰㔞ࢆṧ㒊࡜ẚ㍑

୍᪉ࠊ࢝ࢻ࣑࣒࢘࡟ࡘ࠸࡚ࡣ PGA ࡟ࡼࡾࠊࢪࣕࣀ

ࡍࡿ࡜ࠊࢭ࢖ࣚ࢘࢟ࢬࢱ࡛࢔ࣥࢳࣔࣥ 3㸣ࠊள㖄 40㸣ࣄࢤࡢ᰿㒊࡟ 81.3ppm ࡢ⵳✚ࡀぢࡽࢀࡓࠋࢪࣕࣀࣄ

ᙅࠊࢪࣕࣀࣄࢤ࡛࢔ࣥࢳࣔࣥ 14㸣ࠊள㖄 3㸣࡜࡞ࡗࢤࡢ᰿㒊࡜ởᰁᅵተࡢ PGA ࡢࢫ࣌ࢡࢺࣝࢆᅗ 2 ࡟

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4-4

JAEA-Review 2011-050♧ࡍࠋ⌛⣲ࠊ࢔࣑ࣝࢽ࣒࢘ࠊࢳࢱࣥࠊⅣ⣲ࠊࢡ࣒ࣟࠊ
ࢧ࣐࣒ࣜ࢘࡞࡝ࡢࢩࢢࢼࣝࡀ࡯ࡰᾘ࠼ࠊ࢝ࣝࢩ࣒࢘ࠊ
㕲ࠊ࣒࢝ࣜ࢘ࠊሷ⣲ࠊ࣍࢘⣲ࠊࢼࢺ࣒ࣜ࢘ࡀ࢝ࢻ࣑

㸯㸧ᡞ⏣ᕤᴗ KK㸸ᮅ᪥᪂⪺ 2008.4.18 ᮅห࣒࢘࡜ඹᏑࡋ࡚࠸ࡿࡇ࡜ࡀࢃ࠿ࡿࠋ
⤖ᯝ࡟ᑐࡍࡿホ౯ࡣࡇࢀ࠿ࡽᮏ᱁ⓗ◊✲࡟ධࡿẁ㝵࡛࠶ࡿࡓࡵపࡃ⥅⥆ฟ᮶࡞࠸ࡢࡀṧᛕ࡛࠶ࡿࠋ

㸲㸬ᡂᯝࡢබ⾲ᕝすᖾᏊࠊ㔝ᕝ᠇ኵࠊ⃝ᖭᾈஅࠊ㔝ᮧ㈗⨾ࠕ⎔ቃ࡟㛵ࢃࡿ࣊ࢹࣛᒓ᳜≀࡟ࡘ࠸࡚㸦ࡑࡢ㸰㸧ࢭ࢖ࣚ࢘࢟ࢬࢱ࡟࠾ࡅࡿ࢔ࣥࢳࣔࣥ࠾ࡼࡧள㖄㞟✚ᛶࠖṊⶶ㔝Ꮫ㝔኱Ꮫ◊✲⣖せ ➨㸱㍴
p.37㸫43㸦2006㸧

4-4

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JAEA-Review 2011-050

4-5୰ᏊᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡿ஑ᕞᆅ᪉ࡢⅆᒣάືࢆྵࡴ≀㉁ᚠ⎔ࡢ࢟ࣕࣛࢡࢱࣛ࢖ࢮ࣮ࢩࣙࣥ
Instrumental Neutron Activation Analyses of volcanic rocks from Kyushu island:
Characterization of Material Circulation through Volcanism⇃ᮏ኱Ꮫ ኱Ꮫ㝔⮬↛⛉Ꮫ◊✲⛉ 㛗㇂୰ ฼᫛㸪୕ዲ 㞞ஓ㸪ዉ㡲 㝯ᚿ㸪ୗ㔝 ࡲ࡝࠿㸪ᯞᮧ ᣅஓ㸪㇂⏣ ᗣ௓㸪㛵ཱྀ ᝆᏊ㸪᳃Ọ 㯞⾰Ꮚ㸪㧗Ụ ཭ె㸪ୖᮧ ఙᶞ

1㸬ࡣࡌࡵ࡟
ⅆᒣᒾࡢᚤ㔞ඖ⣲⤌ᡂࡣ㸪࣐ࢢ࣐ࡢ㉳※≀㉁࡟ࡘ
࠸࡚㔜せ࡞᝟ሗࢆ୚࠼࡚ࡃࢀࡿ㸬≉࡟ᾏὒࣉ࣮ࣞࢺ
ࡢỿࡳ㎸ࡳࡀ㛵୚ࡋࡓᓥᘼ㸪኱㝣⦕ࡢⅆᒣᒾ࡜㸪ỿࡳ㎸ࡳࡀ㛵୚ࡋ࡞࠸ᾏὒᓥࡸ኱㝣ෆ㒊࡟⏘ࡍࡿⅆᒣᒾࡣ㸪ࡉࡲࡊࡲ࡞ᚤ㔞ඖ⣲ࡢࣉࣟࢵࢺ࡟࠾࠸࡚᫂░࡟␗࡞ࡿ⤌ᡂࢆ♧ࡋ㸪࣐ࢢ࣐ࡢᡂᅉࡢ㐪࠸ࢆ཯ᫎࡋ
࡚࠸ࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ㸬ᮏ◊✲ᆅᇦ࡛࠶ࡿす༡᪥ᮏᘼ࡟ࡣ㸪ⱝ࠸ᾏὒࣉࣞ
࣮ࢺࡀᓥᘼࡢୗ࡟࠶ࡿ࣐ࣥࢺࣝ࡟ỿࡳ㎸ࢇ࡛࠾ࡾ㸪ྂ࠸ᾏὒࣉ࣮ࣞࢺࡀỿࡳ㎸ࡴᮾ໭᪥ᮏᘼ࡞࡝ࡢᡂ⇍ࡋࡓᓥᘼ࡜ࡣ␗࡞ࡿ≀㉁ᚠ⎔ࡀ㉳ࡇࡗ࡚࠸ࡿࡇ࡜ࡀ
⪃࠼ࡽࢀ࡚࠸ࡿ㸬ࡇࢀࡲ࡛ࡢ◊✲࡛㸪ᓥᘼⓗ࡞ⅆᒣᒾ㸪ᓥᘼⓗ࡞≉ᚩࡀ㠀ᖖ࡟ᑡ࡞࠸ⅆᒣᒾ㸪኱㝣ෆ㒊࡟ぢࡽࢀࡿࡼ࠺࡞࢔ࣝ࢝ࣜ⋞Ṋᒾ㸪ᾏὒࣉ࣮ࣞࢺࡀ
┤᥋ᡂᅉ࡟㛵ࢃࡗࡓ࡜⪃࠼ࡽࢀࡿ࢔ࢲ࢝࢖ࢺࡸ㧗࣐ࢢࢿࢩ࣒࢘Ᏻᒣᒾ࡞࡝ከᵝ࡞࣐ࢢ࣐ࡀάືࡋ࡚࠸ࡿ
ࡇ࡜ࡀศ࠿ࡗ࡚ࡁࡓ㸬ᚤ㔞ඖ⣲ࢆ౑ࡗ࡚࣐ࢢ࣐ࡢᡂ
ᅉࡢ㐪࠸ࢆ⪃࠼ࡿୖ࡛㠀ᖖ࡟⯆࿡࠶ࡿࣇ࢕࣮ࣝࢻ࡛࠶ࡿ㸬 ࡇࢀࡲ࡛㸪஑ᕞᆅ᪉࡟ศᕸࡍࡿⅆᒣᒾࡢ໬Ꮫ⤌ᡂ㸪≉࡟ᚤ㔞ඖ⣲࡟ࡘ࠸࡚ᡃࠎࡢࢢ࣮ࣝࣉࡣ⢭ຊⓗ࡟ㄪᰝ㸪ศᯒࡋ࡚ࡁࡓࡀ㸪 ௒ᅇࡣ஑ᕞࡢⅆᒣࣇࣟࣥࢺ᭱
໭➃࡟఩⨨ࡍࡿጲᓥⅆᒣᄇฟ≀ࡢศᯒ⤖ᯝࢆሗ࿌ࡍࡿ (Fig. 1)㸬
ጲᓥⅆᒣࡣ㸪⣙ 30㹼10 ୓ᖺ๓࡟άືࡋࡓ➨ᅄ⣖ⅆᒣ࡛࠶ࡾ㸪」ᩘࡢ⁐ᒾࢻ࣮࣒࠿ࡽ࡞ࡿ㸬ⅆᒣ┤ୗ࡟ࡣⱝ࠸ࣇ࢕ࣜࣆࣥᾏࣉ࣮ࣞࢺ㸦ᅄᅜᾏ┅㸸⣙ 150 ୓ᖺ๓㸧ࡀỿࡳ㎸ࢇ࡛࠸ࡿ࡜⪃࠼ࡽࢀ࡚࠸ࡿ㸦ఀ⸨㸪
1989㸧㸬ᮏㄽ࡛ࡣጲᓥⅆᒣ࠿ࡽ᥇㞟ࡋࡓⅆᒣᒾᩘヨᩱ࡟ᑐࡋ࡚㸪೫ග㢧ᚤ㙾ほᐹ㸪୺ᡂศ㸪ᚤ㔞ඖ⣲⤌ᡂศᯒࢆ⾜ࡗࡓ⤖ᯝࢆሗ࿌ࡍࡿ㸬 ጲᓥⅆᒣࡢᆅ㉁ࡸᒾ▼࡟ࡘ࠸࡚ࡣఀ⸨㸦1989㸪
1990㸧ࡀヲࡋ࠸ሗ࿌ࢆࡋ࡚࠸ࡿࡀ㸪ᰘ⏣ࡽ㸦2005㸧ࡣ㸪࣐ࢢ࣐ࡢ≉␗࡞⤌ᡂ࡟ὀ┠ࡋ㸪ྠ఩య⤌ᡂࢆሗ࿌ࡋࡓጲᓥ࠾ࡼࡧࡑࡢ㏆ࡃࡢ⏤ᕸᓅ㸪㭯ぢᓅⅆᒣࡢ࣐ࢢ࣐ࡀ㸪୍⯡ⓗ࡞ᓥᘼ࣐ࢢ࣐ࡢᡂᅉ࡜ࡣ␗࡞ࡿ࢔
ࢲ࢝࢖ࢺ࡛࠶ࡿྍ⬟ᛶࢆᣦ᦬ࡋࡓ㸬඾ᆺⓗ࡞ᓥᘼ࡟࠾࠸࡚ࡣ㸪ỿࡳ㎸ࡴᾏὒࣉ࣮ࣞࢺ࡟ྵࡲࢀࡿྵỈ㖔≀ࡀ㧗ᅽ࡛ศゎࡋ࡚⏕ࡌࡓὶయࡀ㸪ᓥᘼୗ࣐ࣥࢺࣝ
࡟௜ຍࡋ㸪ᓥᘼⓗ࡞⤌ᡂࡢ࣐ࢢ࣐ࡀ⏕ࡌࡿ࡜࠸࠺ㄝ
ࡀᗈࡃཷࡅධࢀࡽࢀ࡚࠸ࡿ㸬ࡇࢀ࡟ᑐࡋ࡚ጲᓥ㸪⏤ᕸᓅ㸪㭯ぢᓅ࡟ぢࡽࢀࡿ࣐ࢢ࣐ࡢ⤌ᡂࡣ㸪୍⯡ⓗ࡞ᓥᘼ࣐ࢢ࣐ᡂᅉࡢ௬ㄝ࡛ࡣㄝ࡛᫂ࡁࡎ㸪ỿࡳ㎸ࡴᾏὒࣉ࣮ࣞࢺ⮬యࡀ⁐⼥ࡋ࡚⏕ࡌࡓ࣐ࢢ࣐ࡀ㛵୚ࡋࡓ࢔ࢲ࢝࢖ࢺ࡛࠶ࡿ࡜࠸࠺ࡶࡢ࡛࠶ࡿ㸬ᡃࠎࡣᨺᑕ໬
ศᯒࢆྵࡵࡓᚤ㔞ඖ⣲ࡢ໬Ꮫศᯒ⤖ᯝ࠿ࡽ㸪ࡇࡢ௬ㄝࢆ᳨ドࡋࡓ㸬2㸬ศᯒヨᩱ㸪ศᯒᡭἲ Fig. 1 ஑ᕞࡢ୺࡞➨ᅄ⣖ⅆᒣࡢศᕸᨺᑕ໬ศᯒ⏝ヨᩱࡣḟࡢᡭ㡰࡟ࡼࡗ࡚‽ഛࡋࡓ㸬㸦1㸧ⅆᒣᒾヨᩱࢆ⢊ᮎ໬ࡋ㸪ࡑࢀࡒࢀ⣙ 60 mg ࢆ

JRR-3M PN-1, JRR-4 T ࣃ࢖ࣉ          ᆅ⌫⛉Ꮫヨᩱ࣭ᨺᑕ໬ศᯒ㻙㻌 㻟㻡㻣㻌㻙

JAEA-Review 2011-050⛗㔞㸬㸦2㸧⢊ᮎヨᩱࢆ࣏࢚ࣜࢳ࣭ࣞࣥࣂ࢖࢔ࣝ㸦10mmȭ㸪
20mm L㸧࡟ᤄධ㸬
㸦3㸧ࣁࣥࢲࢦࢸ࡛ࣂ࢖࢔ࣝࡢ⵹ࢆ⼥ᑒ㸬㸦4㸧ࣂ࢖࢔ࣝࢆ࣏࢚ࣜࢳࣞࣥ⿄࡟ධࢀ࡚ࢩ࣮࣮࡛ࣛ
ᑒධ㸬ᨺᑕ໬ศᯒࡢᐇ㦂᮲௳࠾ࡼࡧᡭ㡰ࡣḟࡢ㏻ࡾ࡛࠶
ࡿ㸬JRR-4 ཎᏊ⅔ T ࣃ࢖ࣉ࡛ 100kW ฟຊࡢୗ㸪6 ᫬㛫↷ᑕࡋࡓ㸬JRR-4 ྕ⅔ࡀ౑࠼࡞࠸᫬ࡣ㸪JRR-3 ྕ
⅔ࡢ PN-1 Ẽ㏦⟶࡛ 20 ศ㛫↷ᑕࡋࡓ㸬↷ᑕ୍㐌㛫ᚋ࡟ヨᩱ࢝ࣉࢭࣝࢆ㛤ᑒ㸪࣏࢚ࣜࢳࣞࣥ⿄ࢆ஺᥮ࡋ㸪኱Ꮫ㛤ᨺ◊✲ᐊࡢᐇ㦂฼⏝Ჷ 113㸪115 ᐇ㦂ᐊࡢ࣐࢞ࣥ⥺᳨ฟჾ㸦ASC-20㸧ࢆ⏝࠸࡚▷ᑑ࿨᰾✀ࡢ࣐࢞ࣥ⥺ ᐃࢆ⾜ࡗࡓ㸬ࡲࡓ㸪୍ࣧ᭶ᚋ࡟ࡣ㛗ᑑ࿨᰾✀ࡢ࣐࢞ࣥ⥺ ᐃࢆ⾜ࡗࡓ㸬୺ᡂศඖ⣲࡜࠸ࡃࡘ࠿ࡢᚤ㔞ඖ⣲ྵ᭷㔞ࡣ㸪ྠࡌᒾ▼⢊ᮎヨᩱ࡟ᅄ࣍࢘㓟ࣜࢳ࣒࢘ࡢ⼥๣ࢆຍ࠼࡚㸪ࣅ࣮ࢻ࣭ࢧࣥࣉ࣮࡛ࣛ࢞ࣛࢫࣅ࣮ࢻࢆసᡂࡋ㸪໭஑ᕞ⮬↛ྐ࣭Ṕྐ༤≀㤋ࡢ⺯ග X ⥺ศᯒ⿦⨨㸦ࣇ࢕ࣜࢵࣉࢫ♫〇 PANalytical MagiX PRO㸧ࢆ⏝࠸࡚ศᯒࡋ
ࡓ㸬

Fig. 2 (b) ጲᓥⅆᒣᒾ㢮ࡢ Y-Sr/Y ᅗ (Defant andDrummond, 1990).
 ጲᓥࡣ㯮᭙▼ࡀ⏘ࡍࡿࡇ࡜࡛⪃ྂᏛⓗ࡟ࡶὀ┠ࡉࢀ࡚࠸ࡿࡀ㸪ᅗ 2㸦b㸧࡟࠾࠸࡚ࡣ㸪஑ᕞྛ௚ࡢⅆᒣ࠿ࡽ᥇㞟ࡋࡓ㯮᭙▼㸦ὶ⣠ᒾ㢮㸧ࡢศᯒ್ࡶྜࢃࡏ
࡚ࣉࣟࢵࢺࡋࡓ㸬ጲᓥࡢὶ⣠ᒾࡢࡳࡀ≉␗࡞⤌ᡂࢆ♧ࡍࡇ࡜ࡀ᫂░࡛࠶ࡿ㸬

3㸬ศᯒ⤖ᯝ࣭⪃ᐹ ጲᓥⅆᒣᒾ㢮ࡣ㸪ᩬᬗ㖔≀⤌ྜࡏ࡟ࡼࡗ࡚௨ୗࡢ
2 ࡘࡢࢢ࣮ࣝࣉ࡟኱ูࡉࢀࡿࡇ࡜ࡀศ࠿ࡗࡓ㸬 1㸧ᬑ㏻ゅ㛝▼ (Hb)㸩ᩳ㛗▼ (Pl) ࢆྵࡴࢹ࢖ࢧ࢖
ࢺ࠾ࡼࡧὶ⣠ᒾ㸬 2㸧ࢨࢡࣟ▼ (Grt) ᚤᩬᬗࢆྵࡴὶ⣠ᒾ㸬 ࢢ࣮ࣝࣉ 1 ࡣࢢ࣮ࣝࣉ 2 ࡟ẚ࡭࡚ Sr, Zr ࡟ⴭࡋࡃᐩࡴࡇ࡜ࡀ≉ᚩ࡛࠶ࡿ (Fig. 2a)㸬 ࢢ࣮ࣝࣉ 1 ࡣ Sr/Y ẚࡀ኱ࡁࡃ㸪࢔ࢲ࢝࢖ࢺࡢ㡿ᇦ࡟ධࡿࡀ㸪ࡊࡃࢁ▼ࢆᚤᩬᬗ࡟ྵࡴࢢ࣮ࣝࣉ 2 ⅆᒣᒾ࢔ࢲ࢝࢖ࢺࡢ㡿ᇦ࡟ࡣධࡽ࡞࠸ (Fig. 2b)㸬

Fig. 3 ጲᓥⅆᒣᒾ㢮ࡢᕼᅵ㢮ඖ⣲⤌ᡂ (n-MORB ࡢ್ ࡛ つ ᱁ ໬ ). ͤ n-MORB ࡢ ್ ࡣ Sun and
McDonough (1989) ࢆᘬ⏝㸬࢔ࢲ࢝࢖ࢺࡢ໬Ꮫ⤌ᡂࡣWen et al. (2008) ࢆᘬ⏝ࡋࡓ㸬

Fig. 2 (a) ጲᓥⅆᒣᒾ㢮ࡢᾮ┦⃰㞟ඖ⣲ࣃࢱ࣮ࣥ (ᖹᆒ್ࢆ n-MORB ࡢ್࡛つ᱁໬). ͤ n-MORB ࡢ್ࡣ Sun and McDonough (1989) ࢆᘬ⏝ࡋࡓ㸬 ᕼᅵ㢮ඖ⣲⤌ᡂ࡟ࡘ࠸࡚ࡣ㸪ࢢ࣮ࣝࣉ 1 ࡢὶ⣠ᒾ㸪ࢹ࢖ࢧ࢖ࢺࡀࢢ࣮ࣝࣉ 2 ࡢὶ⣠ᒾ࡟ẚ࡭࡚㍍ᕼᅵ,㔜ᕼᅵࡢ୧᪉࡟ᐩࡴࡇ࡜ࡀࢃ࠿ࡿ (Fig. 3)㸬≉࡟࣮ࣚࣟࢵࣆ࣒࢘ࡢྵ᭷㔞ࡣ୧ࢢ࣮ࣝࣉ㛫࡛኱ࡁࡃ␗࡞ࡿ
(ࢢ࣮ࣝࣉ 1㸼㸼2)㸬
 ୡ⏺ྛᆅ࠿ࡽሗ࿌ࡉࢀࡓ࢔ࢲ࢝࢖ࢺࡢ⤌ᡂ࡜ẚ㍑
ࡍࡿ࡜㸪ࢢ࣮ࣝࣉ 1 ࡢὶ⣠ᒾ㸪ࢹ࢖ࢧ࢖ࢺࡣ࢔ࢲ࢝
࢖ࢺሗ࿌್࡜࡯ࡰྠ➼ࡢ㍍ᕼᅵ㢮ඖ⣲ࡢྵ᭷㔞ࢆ♧ࡍࡀ㸪㔜ᕼᅵ㢮ඖ⣲࡟㛵ࡋ࡚ࡣ࢔ࢲ࢝࢖ࢺሗ࿌್࡜
ẚ࡭࡚ࡸࡸᐩࡴഴྥࡀ࠶ࡿ㸬୍᪉㸪ࢢ࣮ࣝࣉ 2 ࡢὶ⣠ᒾࡣ࢔ࢲ࢝࢖ࢺࡢሗ࿌್࡟ẚ࡭࡚㍍ᕼᅵ㢮ඖ⣲ࡀஈࡋ࠸ࡇ࡜ࡀࢃ࠿ࡿ (Fig. 3)㸬
4-5

㻙㻌 㻟㻡㻤㻌㻙

JAEA-Review 2011-050

4㸬ࡲ࡜ࡵ 㸦1㸧ጲᓥⅆᒣᒾ㢮ࡢ࠺ࡕ㸪ࢢ࣮ࣝࣉ 1 ࡢὶ⣠ᒾ㸪ࢹ࢖ࢧ࢖ࢺࡣグ㍕ᒾ▼Ꮫⓗ≉ᚩ (ᬑ㏻ゅ㛝▼㸩ᩳ㛗▼)㸪ᚤ㔞ඖ⣲ྵ᭷㔞࡜ࡶ࡟ Defant and Drummond(1990) ࡀᐃ⩏ࡋࡓ࢔ࢲ࢝࢖ࢺࡢ≉ᚩࢆ♧ࡋ࡚࠸ࡿ㸬୍᪉㸪ࢢ࣮ࣝࣉ 2 ࡢὶ⣠ᒾࡣグ㍕ᒾ▼Ꮫⓗ≉ᚩ (ࢨࢡࣟ▼ࢆྵࡴࡇ࡜)㸪ᚤ㔞ඖ⣲ྵ᭷㔞࡜ࡶ࡟࢔ࢲ࢝࢖
ࢺࡢ≉ᚩࢆ♧ࡉ࡞࠸ࡇ࡜ࡀࢃ࠿ࡗࡓ㸬 㸦2㸧୧ࢢ࣮ࣝࣉࡢᚤ㔞ඖ⣲ࣃࢱ࣮ࣥࡀ኱ࡁࡃ␗࡞
ࡿࡇ࡜࠿ࡽ㸪୧⪅ࡢ࣐ࢢ࣐ࡢ㉳※≀㉁໬Ꮫ⤌ᡂࡣ␗࡞ࡿྍ⬟ᛶࡀ࠶ࡿ㸬ࢢ࣮ࣝࣉ 1 ࡀ࢔ࢲ࢝࢖ࢺ⤌ᡂࢆ♧ࡍࡇ࡜ࡣ㸪ጲᓥ┤ୗ࡟ỿࡳ㎸ࢇࡔࣇ࢕ࣜࣆࣥᾏࣉ
࣮ࣞࢺ⮬యࡀ㒊ศ⁐⼥ࡋࡓྍ⬟ᛶࢆ♧၀ࡋ࡚࠸ࡿ㸬 㸦3㸧୧ࢢ࣮ࣝࣉࡢ࣐ࢢ࣐ࡀྠࡌᾏὒᆅẆࡢ㒊ศ⁐⼥࡟ࡼࡗ࡚⏕ᡂࡉࢀࡓ࡜௬ᐃࡍࡿ࡜㸪ࢢ࣮ࣝࣉ 2 ࡀࢢ࣮ࣝࣉ 1 ࡟ẚ࡭࡚ Sr, Zr ࡸ㍍ᕼᅵ㢮ඖ⣲㸦≉࡟ Eu㸧࡟ஈࡋ࠸ࡇ࡜ࡣ㸪ࢢ࣮ࣝࣉ 1 ࣐ࢢ࣐⏕ᡂᚋࡢ Sr, Zr,
LREE ࡟ᯤῬࡋࡓᾏὒᆅẆࡢ㒊ศ⁐⼥࡟ࡼࡗ࡚࣐ࢢ
࣐ 2 ࡀ⏕ᡂࡋࡓྍ⬟ᛶࢆ♧၀ࡋ࡚࠸ࡿ㸬୧⪅ࡢᡂᅉ㛵ಀ࡟ࡘ࠸࡚ࡣ௒ᚋࡢㄢ㢟࡛࠶ࡿ㸬 㸦4㸧௨ୖ࡟♧ࡋࡓ࡜࠾ࡾ㸪ᮏ◊✲࡛ᚓࡽࢀࡓ⤖ᯝࡣ㸪஑ᕞ࡟࠾ࡅࡿⅆᡂάື࡟ࡼࡿ≀㉁ᚠ⎔࡟ࡣ࠸ࡃࡘ࠿ࡢ␗࡞ࡗࡓࣃࢱ࣮ࣥࡀ࠶ࡿࡇ࡜ࢆ♧ࡋࡓ㸬ㅰ㎡
 ୰ᛶᏊᨺᑕ໬ศᯒࢆ⾜࠺ୖ࡛ඹྠ฼⏝ᐇ㦂ィ⏬㸪ヨᩱ‽ഛ㸪 ᐃჾ฼⏝࡞࡝࡟࠾࠸࡚⃝ᖭᾈஅẶ㸪ᕝᡭ⛱Ặ㸪▼ᮏග᠇Ặࢆࡣࡌࡵ࡜ࡍࡿ኱Ꮫ㛤ᨺ◊✲ᐊࡢⓙᵝ࡟ࡣᐇ㦂㐙⾜࡟࠶ࡓࡗ࡚ከ኱ࡢ࢔ࢻࣂ࢖ࢫ㸪ࡈ᥼ຓࢆཷࡅࡲࡋࡓ㸬ⓙᵝࡢࢧ࣏࣮ࢺ࡞ࡃࡋ࡚ࡣᮏ
◊✲ࡢ㐙⾜ࡣ㞴ࡋ࠿ࡗࡓ࡜ᛮ࠸ࡲࡍ㸬῝ࡃឤㅰ࠸ࡓ
ࡋࡲࡍ㸬ࡲࡓศᯒ᪉ἲ࡟㛵ࡋ࡚❧ṇ኱Ꮫࡢ⚟ᒸᏕ᫛ᩍᤵ࡟ࡈᩍ♧࠸ࡓࡔࡁࡲࡋࡓ㸬ྜࢃࡏ࡚ឤㅰ࠸ࡓࡋ
ࡲࡍ㸬㸳㸬ᘬ⏝ᩥ⊩
ఀ⸨㡰୍㸪ጲᓥⅆᒣ⩌ࡢᆅ㉁࡜ⅆᒣάື㸪ⅆᒣ ➨ 2 㞟㸪
34㸪1Ѹ17㸪1989㸬ఀ⸨㡰୍㸪ጲᓥⅆᒣ⩌ࡢᒾ▼Ꮫ㸪ᒾ㖔㸪85㸪541-558㸪1990㸬ᰘ⏣ ▱அ㸪ఀ⸨ 㡰୍㸪➉ᮧ ᜨ஧㸪ጲᓥⅆᒣ⩌➨ᅄ⣖ⅆᒣᒾ㢮ࡢ Sr࣭Nd࣭Pb ྠ఩య⤌ᡂ㸪ᆅ⌫ᝨᫍ⛉Ꮫ㛵㐃Ꮫ఍㸪2005 ᖺྜྠ኱఍ண✏㞟㸪J030-003㸪2005㸬
Sun, S.S. and McDonough, W.F., Chemical and isotopic
systematics of oceanic basalts: implications for mantle
composition and processes. In: Saunders, A.D., Norry,
M.D. (Eds.), Magmatism in the Ocean Basins. Geol. Soc.

London. Spec. Publ. 42, 315-345, 1989.
Defant, M.J., Drummond, M.S., Derivation of some modern arc
magmas by melting of young subducted lithosphere. Nature
347, 662-665, 1990.
Wen, D.-R., Chung, S.L., Song, B., Iizuka, Y., Yang, H.-J., Liu,
J. Ji, D. and Gallet, S., Late Cretaceous Gangdese intrusionsof adakitic geochemical characteristic, SE Tibet:
petrogenesis and tectonic implications, Lithos, 105, 1-11,2008.

㸴㸬◊✲ᡂᯝࡢබ⾲Ꮫ఍ㄅ
Miyoshi, M., Shimono, M., Hasenaka, T., Sano, T., Fukuoka, T.,
Determination of boron contents in volcanic rocks byprompt-gamma ray analysis: an application to magma
genesis in Kyushu island, SW-Japan. Journal ofRadioanalytical and Nuclear Chemistry, 278, 343-347,
2008.
Miyoshi, M., Nasu, T., Tajima, T., Kido, M., Mori, Y.,
Hasenaka, T., Shibuya, H., Nagao, K., K-Ar ages ofhigh-magnesian andesite lavas from northern Kyushu,
Japan. Journal of Mineralogical and Petrological Sciences,
103, 183-191, 2008.
Miyoshi, M., Fukuoka, T., Sano, T. and Hasenaka, T.,
Subduction influence of Philippine Sea plate on the
mantle beneath northern Kyushu, SW Japan: an
examination of Boron contents in basaltic rocks. Journalof Volcanology and Geothermal Research, 171, 73-87,
2008.
Sano T, T. Hasenaka, H. Sawahata, T. Fukuoka, Determinationof Ti, K, Sm, and Gd Values in Geological Survey ofJapan Reference Materials by Prompt Gamma Neutron
Activation Analysis, Geostandards and Geoanalytical
Research, 30, 31-36, 2006.
୕ዲ㞞ஓ㸪㛗㇂୰฼᫛㸪᳃ᗣ㸪ᒣୗⱱ㸪㜿⸽࢝ࣝࢹࣛす㒊࡟ศᕸࡍࡿᰣࣀᮌ⁐ᒾ୰࡟ࡳࡽࢀࡿ⤌ᡂ୙ᆒ㉁࡜ࡑ
ࡢᡂᅉ㸬ᒾ▼㖔≀⛉Ꮫ㸪᪥ᮏᒾ▼㖔≀㖔ᗋᏛ఍㸪36㸪
15-29㸪2007㸬୕ዲ㞞ஓ㸪㛗㇂୰฼᫛㸪బ㔝㈗ྖ㸪㜿⸽࢝ࣝࢹࣛᙧᡂᚋ࡟
άືࡋࡓከᵝ࡞࣐ࢢ࣐࡜ࡑࢀࡽࡢᡂᅉ㛵ಀ࡟ࡘ࠸࡚㸬ⅆᒣ㸪᪥ᮏⅆᒣᏛ఍㸪50㸪269-283㸪2005㸬

Ꮫ఍Ⓨ⾲
Miyoshi, M., Shimono, M., Hasenaka, T., Sano, T. andFukuoka, T., Subduction influence of Philippine Sea plateon the mantle beneath Kyushu, SW Japan: An
examination of boron contents in basaltic rocks. IAVCEI
General Assembly, Reykjavik, Iceland, 2008.
Miyoshi, M., Shimono, M., Hasenaka, T., Sano, T. and㻙㻌 㻟㻡㻥㻌㻙

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JAEA-Review 2011-050

Fukuoka, T., Subduction influence of Philippine Sea plateon the mantle beneath Kyushu, SW Japan: An
examination of boron contents in basaltic rocks. 18th
Goldschmidt Conference, Vancouver, Canada, 2008.
᪂ṇ⿱ᑦ㸪ᢡᶫ⿱஧㸪ゅ஭ᮅ᫛㸪⚟ᒸᏕ᫛㸪㛗㇂୰฼᫛㸪బ㔝㈗ྖ㸪℩ᡞෆⅆᒣᒾ㢮ࡢ࣍࢘⣲ྵ᭷㔞㸪ᆅ⌫ᝨᫍ⛉Ꮫ㛵㐃Ꮫ఍㸪2008 ᖺྜྠ኱఍㸪༓ⴥ┴ᖥᙇ࣓ࢵࢭ㸪2008.
㛵ཱྀᝆᏊ㸪㛗㇂୰฼᫛㸪㛗ᒸಙ἞㸪ጸⰋ࢝ࣝࢹࣛᙧᡂ࡟⮳ࡿ๓㥑ⓗ࡞࣐ࢢ࣐άື:࣐ࢢ࣐ΰྜࡢྍ⬟ᛶ㸪᪥ᮏⅆᒣᏛ఍⛅Ꮨ኱఍㸪ᒾᡭ኱Ꮫ㸪2008㸬
Miyoshi, M., Shimono, M., Hasenaka, T., Sano, T., Fukuoka,
T., Furukawa, K., and Shinmura, T., The evolving fluid
flux from the subducting plate beneath Aso area: evidence
from Boron in volcanic products. Cities on Volcanoes 5,
Shimabara, Japan, 2007.
Shimono, M., Miyoshi, T., Fukuoka, T., M., Sano, T. andHasenaka, T., Along-arc variation of Boron data: theinfluence of Philippine Sea plate on the composition of
mantle beneath Kyushu, SW Japan arc. Cities on
Volcanoes 5, Shimabara, Japan, 2007.
Hasenaka, T., Morinaga, M. and Miyoshi, M.,
Kusasenrigahama pumice cone from Aso volcano,
Kyushu, Japan: Petrological characteristics of pumice andcoeval volcanic products representing one of the largest
eruption after caldera-formation, Cities on Volcanoes 5,
Shimabara, Japan, 2007.
㛵ཱྀᝆᏊ㸪㛗㇂୰฼᫛㸪㛗ᒸಙ἞㸪᳃ᗣ㸪ጸⰋ࢝ࣝࢹࣛ࡟
࠾ࡅࡿ 100-29ka ࡢ࣐ࢢ࣐౪⤥ࢩࢫࢸ࣒ࡢኚ㑄㸪ⅆᒣ㒔ᕷᅜ㝿఍㆟ 5㸪ᓥཎ㸪2007㸬
Miyoshi, M., Shimono, M., Hasenaka, T., Sano, T. andFukuoka, T., Determination of boron contents in volcanic
rocks by prompt-gamma ray analysis: an application tomagma genesis in Kyushu island, SW-Japan. 12th
International Conference on Modern Trends in Activation
Analysis (MTAA-12), Tokyo, Japan, 2007.
Miyoshi, M., Shimono, M., Hasenaka, T., Sano, T., Fukuoka, T.
and Shinmura, T., Temporal changes of the subduction
components in volcanic products from Aso area, SW
Japan. 17th Goldschmidt Conference, Koln, Germany,
2007.
Shimono, M., Miyoshi, M., Fukuoka, T., Sano, T. andHasenaka, T., The influence of Philippine Sea plate on thecomposition of mantle beneath Kyushu, SW Japan arc:
Along-arc variation of B data. 17th Goldschmidt
Conference (Koln, Germany, 2007.
Sekiguchi, Y., Hasenaka, T., Nagaoka, S. and Mori, Y.,
Precursory magma activities leading to Airacaldera-forming eruptions in southern kyushu, Japan,
American Geophysical Union, Fall meeting, San
Francisco, 2007.
୕ዲ㞞ஓ㸪ୗ㔝ࡲ࡝࠿㸪㛗㇂୰฼᫛㸪బ㔝㈗ྖ㸪⚟ᒸᏕ᫛㸪໭㒊஑ᕞ⋞Ṋᒾ㢮୰ࡢ࣍࢘⣲ྵ᭷㔞ࡢ᫬㛫ⓗ࣭✵㛫ⓗኚ໬㸬᪥ᮏ㖔≀⛉Ꮫ఍㸪2007 ᖺᗘᖺ఍, ᮾி኱Ꮫ,2007㸬
㛵ཱྀᝆᏊ㸪㛗㇂୰฼᫛㸪㛗ᒸಙ἞㸪᳃ᗣ㸪ጸⰋ࢝ࣝࢹࣛ࡟
࠾ࡅࡿ 100-29ka ࡢᄇฟ≀ࡢᒾ▼Ꮫⓗ≉ᚩ㸪ᆅ⌫ᝨᫍ⛉Ꮫ㛵㐃Ꮫ఍㸪2007 ᖺྜྠ኱఍㸪༓ⴥ┴ᖥᙇ࣓ࢵࢭ㸪
2007.
Miyoshi, M., Shimono, M., Fukuoka, T., Sano, T., Hasenaka, T.,
Slab influence of hot Philippine Sea plate on the subarc
mantle: An examination of Boron contents in basaltic
rocks from northern Kyushu, SW Japan, 16th
Goldschmidt conference, Melbourne, Australia, 2006.
Shimono, M., Miyoshi, M., Fukuoka, T., Sano, T. andHasenaka, T., Temporal and spatial influence ofPhilippine Sea plate on the composition of basaltic rocks
from southern Kyushu, SW Japan arc -- a study fromboron analysis, 16th Goldschmidt conference, Melbourne,
Australia, 2006.
୕ዲ㞞ஓ㸪ୗ㔝ࡲ࡝࠿㸪⚟ᒸᏕ᫛㸪బ㔝㈗ྖ㸪㛗㇂୰฼᫛㸪ࣇ࢕ࣜࣆࣥᾏࣉ࣮ࣞࢺࡢỿࡳ㎸ࡳࡀ໭㒊஑ᕞࡢࢯ࣮
ࢫ࣐ࣥࢺࣝ࡟୚࠼ࡓᙳ㡪㸫ⅆᒣᒾࡢ࣍࢘⣲ྵ᭷㔞ࢆ⏝࠸ࡓ᳨ウ㸫㸬᪥ᮏⅆᒣᏛ఍㸪 2006 ᖺᗘ⛅Ꮨ኱఍㸪⇃ᮏ┴㜿⸽㸪2006㸬ୗ㔝ࡲ࡝࠿㸪୕ዲ㞞ஓ㸪⚟ᒸᏕ᫛㸪బ㔝㈗ྖ㸪㛗㇂୰฼᫛㸪
2006㸬஑ᕞ༡㒊࡟⏘ࡍࡿⅆᒣᒾ㉳※≀㉁୰ࡢ࣍࢘⣲ྵ᭷㔞ࡢ✵㛫ⓗ࣭᫬㛫ⓗኚ໬㸬᪥ᮏⅆᒣᏛ఍㸪2006ᖺᗘ⛅Ꮨ኱఍㸪⇃ᮏ┴㜿⸽㸪2006㸬
Miyoshi, M., Shimono, M., Fukuoka, T., Sano, T. andHasenaka, T., Subduction metasomatism beneath northern
Kyushu: an examination from spatial and temporalvariations of boron contents in basalts. ᆅ⌫ᝨᫍ⛉Ꮫ㛵㐃Ꮫ఍㸪2006 ᖺྜྠ኱఍㸪༓ⴥ┴ᖥᙇ࣓ࢵࢭ㸪2006㸬ୗ㔝ࡲ࡝࠿㸪୕ዲ㞞ஓ㸪⚟ᒸᏕ᫛㸪బ㔝㈗ྖ㸪㛗㇂୰฼᫛㸪஑ᕞ༡㒊࡟⏘ࡍࡿⅆᒣᒾ㉳※≀㉁࡬ࡢࣇ࢕ࣜࣆࣥᾏ
ࣉ࣮ࣞࢺࡢᐤ୚࡟ࡘ࠸࡚㹼࣍࢘⣲ࢆ⏝࠸ࡓ◊✲㸪ᆅ⌫ᝨᫍ⛉Ꮫ㛵㐃Ꮫ఍㸪2006 ᖺྜྠ኱఍㸪༓ⴥ┴ᖥᙇ࣓ࢵࢭ㸪2006.
Miyoshi, M., Shimono, M., Fukuoka, T., Sano, T. andHasenaka, T., Spatial and temporal variations of Boroncontents of basaltic rocks from northern Kyushu, SW
Japan arc. American Geophysical Union, fall meeting,
San Francisco, USA, 2005.
㧗Ụ཭ె㸪ዉ㡲㝯ᚿ㸪㛗㇂୰฼᫛㸪㛤⪺ᓅⅆᒣ⁐ᒾ⤌ᡂࡢᖺ௦ኚ໬࠿ࡽ᥎ᐃࡋࡓ࣐ࢢ࣐⁀ࡲࡾ࡛ࡢ㐣⛬㸪ᆅ⌫ᝨᫍ⛉Ꮫ㛵㐃Ꮫ఍㸪2005 ᖺྜྠ኱఍㸪༓ⴥ┴ᖥᙇ㸪
2005㸬

㻙㻌 㻟㻢㻜㻌㻙

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JAEA-Review 2011-050

4-6

㓟ᛶ Ἠ࿘㎶ᆅᇦ࡟࠾ࡅࡿࣄ⣲ືែㄪᰝ
Origin and fate of arsenic in volcanic hot spring areaᮌᕝ⏣႐୍㸪኱஭㝯ኵ㸪᪩ὠᓅᏹ㸪బ㔝῟Ꮚ㸪஭ୖ⥤㸪ᑠ⏣ᖾᖹ㸪⸨ᏹஅ㸪኱㔝᭷ᕼᏊ㸪
ிච㈼୍㸪బ⸨┤Ꮚ 㸦ୖᬛ኱Ꮫ⌮ᕤᏛ㒊໬Ꮫ⛉㸧
Yoshikazu Kikawada, Takao Oi, Takehiro Hyatsu, Junko Sano, Aya Inoue, Kohei Oda,
Hiroyuki Fuji, Yukiko Ohno, Ken-ichi Kyomen, Naoko Sato
(Department of Chemistry, Faculty of Science and Technology, Sophia University)ᇦࡢ※Ἠ㉳※ࡢࣄ⣲ࡀ⎔ቃ୰ࢆ࡝ࡢࡼ࠺࡟⛣ື㸪㸯㸬◊✲ࡢ⫼ᬒ࡜┠ⓗࣄ⣲ࡣẘᛶࢆ᭷ࡍࡿඖ⣲࡜ࡋ࡚♫఍ⓗ࡟ᗈࡃ㐠ᦙࡉࢀ࡚࠸ࡿࡢ࠿ࢆྍ⬟࡞㝈ࡾᐃ㔞ⓗ࡟ồࡵ㸪▱ࡽࢀ࡚࠸ࡿࡀ㸪ᐇ㝿࡟ࡣ≉ู࡞ඖ⣲࡛ࡣ࡞ࡃ㸪ᙜヱᆅᇦ࡟࠾ࡅࡿࣄ⣲ࡢືែࢆ᫂ࡽ࠿࡟ࡍࡿࡇ

ᕤᴗⓗ࡟ྂࡃ࠿ࡽ⏝࠸ࡽࢀ㸪⌧ᅾ࡟࠾࠸࡚ࡶ༙ᑟ

࡜ࢆ┠ⓗ࡜ࡋࡓ㸬యᮦᩱ࡜ࡋ࡚฼⏝ࡉࢀࡿ࡞࡝㸪⌧௦♫఍࡟ࡣḞࡃࡇ࡜ࡢ࡛ࡁ࡞࠸ඖ⣲࡛࠶ࡿ㸬ⅆᒣᆅᇦ࡟ࡣࡈࡃᬑ
㏻࡟ࣄ⣲ࡀᏑᅾࡋ࡚࠾ࡾ㸪ⅆᒣᛶ

㸰㸬ⲡὠ
ⲡὠ

Ἠࡢ୰࡟ࡶ┦

ἨᆅᇦࡢᴫせἨࡣ⩌㤿┴໭す㒊㸪ⲡὠⓑ᰿ⅆᒣࡢᮾ㯄ᙜ㔞ࡢࣄ⣲ࢆྵࡴࡶࡢࡀᏑᅾࡍࡿ㸬ࡓ࡜࠼ࡤ㸪⛅࡟఩⨨ࡍࡿ㸪᪥ᮏࢆ௦⾲ࡍࡿ⏣┴ࡢ⋢ᕝἨ࡛ࡣ㸪ࡑࡢ※ἨỈࡀὶୗࡍࡿἙᕝ

ᆅᇦෆ࡟ࡣከࡃࡢ※Ἠࡀ‪ฟࡍࡿࡀ㸪ࡑࡢ࠸ࡎࢀ

࡟࠾࠸࡚㸪ࣄ⣲໬ྜ≀ࢆྵࡴỿẊ≀ࡀㄆࡵࡽࢀ࡚

ࡶࡀᙉ㓟ᛶ࡛࠶ࡿ㸬ᆅᇦෆࡢ௦⾲ⓗ※Ἠ࡜ࡑࡢ

࠸ࡿ[1]㸬

pH ࢆᅗ 1 ࡟♧ࡍ㸬ࡇࡢ୰࡛㸪୓௦㖔※Ἠ(BND)ᡃࠎࡣࡇࢀࡲ࡛ࡢ◊✲࡛㸪⩌㤿┴ⲡὠἨᆅᇦἨࡢࡦ࡜ࡘ࡛࠶ࡿ㸬࡜ⲡὠ‫※⏿‮‬Ἠ(KYB)ࡢ 2 ※Ἠ࡟ࡼࡾ㸪ⲡὠࡢ୓௦㖔※Ἠࡀ㸪1990 ᖺ௦ᚋ༙௨㝆㸪10 ppm ๓ࡢᚋࡢ㧗࠸ࣄ⣲⃰ᗘ࡟࠶ࡾ㸪ࡑࡢᖺ㛫ࣄ⣲౪⤥㔞ࡀࡽࢀ࡚࠸ࡿ㸬

ἨἨ⾤࡛฼⏝ࡉࢀࡿ※ἨỈࡢ࡯࡜ࢇ࡝ࡀ༨ࡵ

50 ࢺࣥ㏆ࡃ࡟ࡶ㐩ࡍࡿࡇ࡜ࢆ᫂ࡽ࠿࡟ࡋࡓ[2]㸬

ᆅᇦෆ࡛᭱኱ࡢ‪ฟ㔞ࢆ᭷ࡍࡿ୓௦㖔※Ἠࡣ㸪ࡇࡢ኱㔞ࡢ※Ἠ㉳※ࡢࣄ⣲ࡣ㸪᭱⤊ⓗ࡟ࡣᆅᇦෆ

1970 ᖺ࡟◲㯤㖔ᒣࡢ᥀๐୰࡟ᆙ㐨ෆࡼࡾ‪ฟࢆࡢἙᕝ࡬࡜ὶධࡋ㸪ᇦእ࡬࡜㐠ᦙࡉࢀࡿ㸬ⲡὠ㛤ጞࡋࡓẚ㍑ⓗ᪂ࡋ࠸※Ἠ࡛࠶ࡿ㸬୓௦㖔※Ἠࡢ

Ἠࡢ※Ἠࡣࡑࡢࡍ࡭࡚ࡀᙉ㓟ᛶ࡛࠶ࡿࡇ࡜࠿ࡽ㸪※ἨỈࡣᘬ‫ࡾࡼ࡟ࣉ࢖ࣃ‮‬ࡑࢀࡽࡀὶධࡍࡿἙᕝࡣ㓟ᛶἙᕝ࡛࠶ࡾ㸪௒᪥㸪ࡀ㸪ᮍ฼⏝※ἨỈࡢ୍㒊ࡣ㸪※Ἠ‪ฟཱྀ㏆ࡃ࡟タ

ᅜᅵ஺㏻┬࡟ࡼࡿἙᕝ୰࿴஦ᴗࡀ⾜ࢃࢀ࡚࠸ࡿ㸬ࡅࡽࢀࡓᨺฟụ㸪࡞ࡽࡧ࡟ᇦෆࡢἙᕝ࡬┤᥋ᨺฟࡋࡓࡀࡗ࡚ἙᕝỈࡢ୰࿴ࡀࡇࡢᆅᇦࡢࣄ⣲ࡢᣲࡉࢀ࡚࠸ࡿ[3]㸬
ⲡὠື࡟኱ࡁ࡞ᙳ㡪ࢆ୚࠼࡚࠸ࡿࡇ࡜ࡣ㛫㐪࠸࡞࠸㸬ᮏ◊✲࡛ࡣ㸪ࡇࡢࡼ࠺࡞⫼ᬒࡢࡶ࡜㸪ⲡὠἨᆅἨ⾤࡟౪⤥ࡉࢀࡿ

Ἠࡀ఩⨨ࡍࡿⲡὠⓑ᰿ᒣᮾ㯄࡟ࡣ㸪‫‮‬ᕝỈ⣔࡟ᒓࡍࡿ 3 ࡘࡢἙᕝ㸪ࠕ኱ἑᕝࠖ㸪ࠕ㇂ἑᕝࠖ
㸪

JRR-3 PN-1, PN-2 ; JRR-4 T-pipe, S-pipe㸪 ᆅ⌫໬Ꮫⓗヨᩱᨺᑕ໬ศᯒ㻙㻌 㻟㻢㻝㻌㻙

JAEA-Review 2011-050

ࠕ‫‮‬ᕝࠖࡀᏑᅾࡋ(ᅗ 1)㸪ࡑࡢ࠸ࡎࢀࡶࡀᙉ㓟ᛶ⣬ࢆ⏝࠸࡚ℐ㐣ࡋࡓ㸬ࡲࡓ୍㒊ࡢヨᩱ࡟ࡘ࠸࡚ࡣ㸪ࡢἨỈ࡞ࡽࡧ࡟‪Ỉࡢὶධ࡟ࡼࡾ㓟ᛶࡢἙᕝ⁐Ꮡࡍࡿࣄ⣲ࡢ໬Ꮫᙧែࢆ᥎ᐹࡍࡿࡓࡵ㸪ࣆࣟࣜ࡜࡞ࡗ࡚࠸ࡿ㸬ࡇࡢ୰࡛‫‮‬ᕝࡣ㸪୓௦㖔※Ἠ㸪ⲡࢪࣥࢪࢳ࢜࢝ࣝࣂ࣑ࣥ㓟(PDC)ඹỿἲ[4] ࢆ⏝࠸ὠ‫※⏿‮‬Ἠ࡟ຍ࠼㸪 Ἠ⾤࡟‪ฟࡍࡿᑠつᶍ࡞※ࡓ As(III)࡜ As(V)ࡢศูᐃ㔞ࢆヨࡳࡓ㸬Ἠ࠿ࡽࡢᮍ฼⏝※ἨỈࢆ㞟Ỉࡋ㸪ࡉࡽ࡟ࡣἨ⾤ヨᩱỈ୰ࡢ඲⁐Ꮡࣄ⣲⃰ᗘࡣ㸪ヨᩱỈࢆℐ⣬ࡢ࡛ࡢ฼⏝ᚋࡢᗫ‫ⲡ࡚ࡏేࡶࢆ‮‬ὠἨ⾤ᑠ∦࡟ྵᾐࡉࡏ㸪ࡇࢀࢆ↷ᑕヨᩱ࡜ࡋ࡚୰ᛶᏊᨺ

Ἠࡢ୰ᚰ㒊ࢆὶࢀ࡚࠸ࡿ㸬‫‮‬ᕝỈ⣔࡛ࡣᅜᅵ஺㏻┬࡟ᑕ໬ศᯒἲ࡟ࡼࡾᐃ㔞ࡋࡓ㸬ࡲࡓ୍㒊࡟ࡘ࠸࡚ࡣ㸪ࡼࡿἙᕝ୰࿴஦ᴗࡀ⾜ࢃࢀ࡚࠾ࡾ㸪3 Ἑᕝࡢࡍ࡭

Ỉ⣲໬≀Ⓨ⏕ἲ࡟ࡼࡿཎᏊ྾ගศගἲࡶే⏝ࡋ࡚࡟࠾࠸࡚▼⅊ஙᾮࡢ୰࿴๣ࡀᢞධࡉࢀ࡚࠸ࡿ㸬ࡓ㸬PDC ඹỿἲ࡛ࡣ㸪᥇Ỉ┤ᚋ࡟ヨᩱỈ࡟࢔ࣥࣔ୰࿴๣ࢆᢞධࡉࢀࡓ࠶࡜ࡢ 3 Ἑᕝࡣ㸪୰࿴ỿẊ≀ࢽ࣒࢘ࣆࣟࣜࢪࣥࢪࢳ࢜࢝ࣝࣂ࣑ࣥ㓟(APDC)࡜

ࡢᤕ㞟࡜୰࿴ࡢಁ㐍ࢆ┠ⓗ࡜ࡋ࡚సࡽࢀࡓရᮌ

◪㓟㖄ࢆຍ࠼㸪⏕ࡌࡓ Pb(PDC)2 ࡢỿẊࢆ࣓ࣥࣈࢲ࣒࡟࠾࠸࡚ྜὶࡍࡿ㸬ရᮌࢲ࣒࠿ࡽࡣ㏦Ỉ⟶ࢆࣛࣥࣇ࢕ࣝࢱ࡟ࡼࡾࢁูᅇ཰ࡋࡓ㸬ࡇࡢ

㏻ࡋ࡚‫‮‬ᕝⓎ㟁ᡤ࡟㏦ࡽࢀ㸪ⓑ◁ᕝ࡟ྜὶࡍࡿ㸬Pb(PDC)2 ࡟ࡣ As(III)ࡀ㑅ᢥⓗ࡟ඹỿࡍࡿ㸬ᅇ཰ⓑ◁ᕝࡣ࿃ጔᕝ࡟ྜὶࡋ㸪᭱⤊ⓗ࡟ࡣ฼᰿ᕝ࡬࡜

ࡋࡓ Pb(PDC)2 ࡢỿẊࡣ㠀◚ቯ୰ᛶᏊᨺᑕ໬ศᯒ

⧅ࡀࡗ࡚࠸ࡿ㸬ἲ ࡟ ౪ ࡋ 㸪ᚓ ࡽ ࢀ ࡓ ࣄ⣲ ⃰ ᗘ ࠿ ࡽヨ ᩱ Ỉ ୰ ࡢ
As(III)⃰ᗘࢆồࡵ㸪඲ࣄ⣲⃰ᗘ࠿ࡽ As(III)⃰ᗘࢆᕪࡋᘬࡃࡇ࡜࡛ As(V)⃰ᗘࢆồࡵࡓ㸬ヨᩱỈࡢỈ㸪pH ࡣ᥇Ỉ᫬࡟ᐃࡋ㸪୺せᡂ

ศ⃰ᗘࡣ⅖ගගᗘἲ㸪ICP Ⓨගศᯒἲ㸪࢖࢜ࣥࢡ࣐ࣟࢺࢢࣛࣇ࢕࣮࡟ࡼࡾᐃ㔞ࡋࡓ㸬ᅗ ⲡὠ

Ἠᆅᇦࡢ※ἨỈ࡜ἙᕝỈࡢ S+‫ࡣە‬ᆅᇦෆࡢ୺せ※Ἠࢆ♧ࡍ㸬㸱㸬ヨᩱࡢ᥇ྲྀ࡜ศᯒ
3.1

ἨỈ࡞ࡽࡧ࡟ἙᕝỈヨᩱୖᬛ኱Ꮫ⌮ᕤᏛ㒊໬Ꮫ⛉࡟ಖᏑࡉࢀ࡚࠸ࡿ㸪
1964 ᖺ௨㝆ࡢ‫‮‬ᕝࡢ୰࿴๓ヨᩱỈࢆศᯒ࡟౪ࡋ
ࡓ㸬๓㏙ࡢ㏻ࡾ㸪‫‮‬ᕝࡣ୓௦㖔※ἨỈࡀὶධࡍࡿ
Ἑᕝ࡛࠶ࡿ㸬ࡉࡽ࡟㸪ⲡὠἨᆅᇦࡢ※ἨỈ࡞ࡽࡧ࡟‫‮‬ᕝࡢἙᕝỈࢆ᪂ࡓ࡟᥇ྲྀࡋ㸪ࡇࢀࡶศᯒ࡟
౪ࡋࡓ㸬ἙᕝỈ࡟ࡘ࠸࡚ࡣ୰࿴๣ࡢᢞධ๓࡜ᢞධᅗ ἙᕝỈヨᩱࡢ᥇ỈᆅⅬ‫※ࡣە‬ἨỈ㸪‫ࡣۑ‬ἙᕝỈࡢ᥇ỈᆅⅬࢆ♧ࡍ㸬Ἑᕝ᥇Ỉ
ᆅⅬ࡟௜ࡉࢀࡓ͆$͇ࡣ୰࿴ᚋ㸪͆%͇ࡣ୰࿴๓ࢆࡑࢀ
ࡒࢀ♧ࡍ㸬‫ࡣۼ‬Ἑᕝ୰࿴ᆅⅬࢆ♧ࡍ㸬

3.2 Ἑᕝ୰࿴⏕ᡂ≀ᚋ࡟࠾࠸࡚ࡑࢀࡒࢀ᥇ྲྀࡋࡓ(ᅗ 2)㸬୰࿴ᚋࡢἙ

ἙᕝỈࡢ୰࿴ᚋ࡟⏕ࡌࡿ୰࿴⏕ᡂ≀࡟ྵࡲࢀᕝỈࡢሙྜ㸪୰࿴๣࡜୰࿴⏕ᡂ≀࡟ࡼࡾ⃭ࡋࡃᠱࡿࣄ⣲㔞ࢆồࡵࡿࡓࡵ㸪Ἑᕝ୰࿴⏕ᡂ≀ࢆ᥇ྲྀࡋ⃮ࡋ࡚࠸ࡿࡓࡵ㸪࢔ࢻࣂࣥࢸࢵࢡᮾὒࡢ No. 2 ℐࡓ㸬୰࿴ᚋࡢᠱ⃮≀ࢆྵࡴἙᕝỈࢆ㸪Ꮝᚄ 0.45 ȣ㻙㻌 㻟㻢㻞㻌㻙

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JAEA-Review 2011-050

m ࡢ࣓ࣥࣈࣛࣥࣇ࢕ࣝࢱࢆ⏝࠸࡚྾ᘬℐ㐣ࡋ㸪ࣇ㸲㸬⤖ᯝ࡜⪃ᐹ࢕ࣝࢱୖ࡟ᤕ㞟ࡉࢀࡓᠱ⃮≀ࢆᅇ཰ࡋࡓ㸬ࡲࡓἙ

4.1 ‫‮‬ᕝࡢ⁐Ꮡࣄ⣲⃰ᗘࡢ⤒ᖺኚ໬ᗋ࡟ỿ╔ࡋࡓ〓Ⰽࡢ୰࿴⏕ᡂ≀ࢆ᥇ྲྀࡋࡓ㸬ᅗ 3 ࡟ࡣ㸪‫‮‬ᕝࡢ୰࿴๓ࡢ⁐Ꮡࣄ⣲⃰ᗘࡢ⤒ᖺࣇ࢕ࣝࢱ࡟ࡼࡾᅇ཰ࡋࡓᠱ⃮≀㸪࡞ࡽࡧ࡟⢊○ኚ໬ࢆ㸪୓௦㖔※Ἠࡢ⁐Ꮡࣄ⣲⃰ᗘ⤒ᖺኚ໬࡜࡜

ࡋࡓἙᗋỿ╔≀ࡣ㸪㠀◚ቯ୰ᛶᏊᨺᑕ໬ศᯒἲ࡟

ࡶ࡟♧ࡍ㸬ࡇࢀࢆぢࡿ࡜㸪‫‮‬ᕝࡢࣄ⣲⃰ᗘࡢ⤒ᖺࡼࡾࣄ⣲⃰ᗘࢆồࡵࡓ㸬ࡲࡓ㸪Ἑᗋỿ╔≀࡟ࡘ࠸ኚ໬ࡣ୓௦㖔※Ἠࡢࣄ⣲⃰ᗘࡢ⤒ᖺኚ໬࡜┦ఝ࡚ࡣࣇࢵ໬Ỉ⣲㓟࡟ࡼࡾศゎ㸪⁐ᾮ໬ࡋ㸪⅖ගගⓗ࡛࠶ࡾ㸪‫‮‬ᕝࡢࣄ⣲⃰ᗘࡣ୓௦㖔※Ἠ࠿ࡽࡢὶᗘἲ㸪ICP Ⓨගศᯒἲ࡟ࡼࡾ୺せᡂศࡢᐃ㔞ࢆ⾜ධỈ࡟᏶඲࡟ᨭ㓄ࡉࢀ࡚࠸ࡿ㸬࠺࡜࡜ࡶ࡟㸪᩿㠃ࡢ EPMA ศᯒ࡞ࡽࡧ࡟㸪X ⥺3.3 ᅵተヨᩱⲡὠ Ἠᆅᇦࡢྛᡤ࠿ࡽ㸪ࢫࣃ࢖ࣛࣝࢹ࢕࣮࢞
ࡶࡋࡃࡣࣆ࣮ࢺࢥ࢔ࢧࣥࣉ࣮ࣛࢆ⏝࠸࡚ᅵተヨᩱࢆ᥇ྲྀࡋࡓ㸬ࢫࣃ࢖ࣛࣝࢹ࢕࣮࢞ࢆ⏝࠸ࡓሙྜ࡟ࡣᆅ⾲ୗ 10 cm ௨ୗࡢᅵተࢆ㸪ࡲࡓ㸪ࢥ࢔ࢧࣥࣉ࣮ࣛࢆ⏝࠸ࡓሙྜ࡟ࡣ㸪ᚓࡽࢀࡓᆅ⾲ୗ 30 cm

Concentration of arsenic (mg/L)⢊ᮎᅇᢡ(XRD)࡟ࡼࡿ໬Ꮫ✀ࡢྠᐃࢆヨࡳࡓ㸬

12

(a)

8
4
0
2

(b)

1

0

ࡲ࡛ࡢࢥ࢔ヨᩱࢆᩘ cm ࡈ࡜࡟ศ๭ࡋ࡚௨ᚋࡢ
ศᯒ࡟౪ࡋࡓ㸬ࣄ⣲⃰ᗘࡣ㠀◚ቯ୰ᛶᏊᨺᑕ໬ศᯒἲ࡟ࡼࡾ
ồࡵ㸪୺せᡂศ⃰ᗘࡣࣇࢵ໬Ỉ⣲㓟࡟ࡼࡾศゎ㸪

1980

1990
Year

2000

ᅗ  ⁐Ꮡࣄ⣲⃰ᗘࡢ⤒ᖺኚ໬D ࡣ୓௦㖔※ἨỈ㸪 E ࡣ‫‮‬ᕝࡢ୰࿴๓ࡢἙᕝỈ㸬⁐ᾮ໬ࡋ࡚㸪⅖ගගᗘἲ㸪ICP Ⓨගศᯒἲ㸪࢖࢜ࣥࢡ࣐ࣟࢺࢢࣛࣇ࢕࣮࡟ࡼࡾᐃ㔞ࡋࡓ㸬ࡲࡓ XRD

1970

4.2 ἙᕝỈ୰ࡢࣄ⣲⃰ᗘ࡜ࣄ⣲㐠ᦙ㔞
⾲ 1㸪2 ࡟㸪‫‮‬ᕝỈ⣔ࡢ 3 Ἑᕝ࡟࠾ࡅࡿࣄ⣲⃰࡟ࡼࡿ㖔≀✀ࡢྠᐃࢆヨࡳࡓ㸬ᗘࡢศᯒ⤖ᯝࢆἙᕝὶ㔞[6]࡜࡜ࡶ࡟♧ࡍ㸬⾲ 1 ࠿ࡽ㸪୰࿴๓ࡢἙᕝ࡛ࡣ‫‮‬ᕝࡢ⁐Ꮡࣄ⣲⃰ᗘࡀ᭱ࡶ

3.4 ୰ᛶᏊᨺᑕ໬ศᯒࡢᐇ㝿୰ᛶᏊᨺᑕ໬ศᯒࡣ᪤ሗࡢᡭ㡰࡟๎ࡗ࡚⾜ࡗ㧗ࡃ㸪᭱኱ 3 mg/L ࡟㐩ࡋ࡚࠸ࡿ㸬⁐Ꮡࣄ⣲⃰ᗘ

ࡓ[5]㸬ᾮయヨᩱ࡟ࡘ࠸࡚ࡣ㸪0.5 mL ࢆℐ⣬࡟ྵ࡜Ἑᕝὶ㔞࠿ࡽྛἙᕝࡢࣄ⣲㐠ᦙ㔞ࢆぢ✚ࡶࡿᾐࡉࡏࡓࡶࡢࢆ㸪ࡲࡓᅛయヨᩱ࡟ࡘ࠸࡚ࡣᩘ㹼ᩘ࡜(⾲ 1)㸪‫‮‬ᕝࡢࣄ⣲㐠ᦙ㔞ࡀᅽಽⓗ࡟㧗ࡃ㸪ᖺ

10 mg ࢆ⢭⛗ࡋࡓࡶࡢࢆ࣏࢚ࣜࢳࣞࣥࣂࢵࢢ࡟஧

㛫 28 ࢺࣥ࡜ぢ✚ࡶࡽࢀࡓ㸬ࡇࢀࡣࡇࡢᆅᇦࡢἙ

㔜࡟ᑒධࡋ࡚↷ᑕヨᩱ࡜ࡋࡓ㸬ẚ㍑ᶆ‽ヨᩱ࡜ࡋᕝ࡟ࡼࡾ㐠ᦙࡉࢀࡿࣄ⣲ࡢ 99㸣ࢆ༨ࡵ࡚࠸ࡿ㸬୍࡚ࡣ㸪ཎᏊ྾ග⏝ࣄ⣲ᶆ‽⁐ᾮࢆℐ⣬࡟ྵᾐࡉࡏ

᪉㸪୰࿴ᚋࡢἙᕝࡢࣄ⣲⃰ᗘࡣ࠸ࡎࢀࡶ᳨ฟ㝈⏺

ࡓࡶࡢࢆྠ᫬↷ᑕࡋࡓ㸬୰ᛶᏊ↷ᑕࡣ JRR-3 ࡢᮍ‶(< 0.01 mg/L)࡛࠶ࡗࡓ(⾲ 2)㸬ࡋࡓࡀࡗ࡚㸪

PN-1㸪PN-2㸪ࡶࡋࡃࡣ JRR-4(ᐃ᱁ฟຊ)ࡢ T ࣃ୰࿴๓ࡢἙᕝỈ࡟ྵࡲࢀ࡚࠸ࡓࣄ⣲ࡢ࡯࡜ࢇ࡝

࢖ࣉ㸪S ࣃ࢖ࣉࢆ⏝࠸࡚ 3 ศ࠿ࡽ 5 ศ㛫↷ᑕࡋ㸪ࡀἙᕝ୰࿴࡟ࡼࡗ࡚⏕ࡌࡿ୰࿴⏕ᡂ≀࡟ᤕ㞟ࡉ෭༷᫬㛫 1 ᪥㸪ᩘ 1000 ⛊ࡢࢀ㸪ᠱ⃮ែ࡜࡞ࡗ࡚Ἑᕝࢆὶୗࡋ࡚࠸ࡿࡇ࡜ࢆពᨺ◊✲ᐊࡢᐃ᫬㛫࡛㸪኱Ꮫ㛤ᐃჾࢆ฼ ⏝ࡋ࡚࣐࢞ࣥ⥺ࢫ࣌ࢡࢺ࿡ࡍࡿ㸬࣓ࣟࢺࣜࢆᐇ᪋ࡋࡓ㸬㻙㻌 㻟㻢㻟㻌㻙

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⾲1 ୰࿴๓䛾ἙᕝỈ䛾⁐Ꮡ䝠⣲⃰ᗘ䛸䝠⣲㐠ᦙ㔞䛾ぢ✚䜒䜚⤖ᯝ

Sampling location(mg /L)
30-Nov-2004
0.08
30-Nov-2004
3.04
30-Nov-2004
1.29
Yu River29-Jul-2004
1.95
30-Nov-2004
1.37
YU-B4
4-Jun-2005
1.55
27-Jul-2005
1.51
29-Jul-2004
ND
Yazawa River YZ-B
27-Jul-2005
0.01
2-Aug-2004
0.32
OS-B1
Osawa River
2-Aug-2005
0.19
OS-B2
2-Aug-2005
0.03* Data cited from Hirabayashi and Mizuhashi [6]Amount ofarsenictransported⣲⃰ᗘࢆồࡵࡿ࡜㸪ᠱ⃮ែࢆࡶྵࡵࡓ඲ࣄ⣲⃰ᗘ[Ave.] (L /min)(ton /year)ࡣ 0.12 mg/L ࡛࠶ࡗࡓ㸬௬࡟ရᮌࢲ࣒࡟ὶධࡍࡿ

YU-B1
YU-B2
YU-B3

-

3 ࡘࡢἙᕝࡢྜィὶ㔞࡜㸪‫‮‬ᕝⓎ㟁ᡤࢆ௓ࡋ࡚ⓑ◁ᕝ࡟ὶධࡍࡿỈ㔞࡜ࡀ➼ࡋ࠸࡜ࡍࡿ࡞ࡽࡤ㸪ⓑ(1.60)

33000

28(0.01)

8800

0.05(0.26)

10000◁ᕝ࡟ࡣᖺ㛫⣙ 3 ࢺࣥࡢࣄ⣲ࡀὶධࡍࡿࡇ࡜࡟࡞
ࡿ㸬ࡇࢀࡀⲡὠ

Sampling date≀ࡸὶධᅵ◁ࡢሁ✚࡟ࡼࡿ࣮࢜ࣂ࣮ࣇ࣮ࣟࢆ㑊

0.16

ࡅࡿࡓࡵ㸪ᐃᖖⓗ࡟ࢲ࣒ෆࡢὼ

YU-A1
YU-A2

Yazawa River

YZ-A

Osawa River

OS-A
SKD

Shinaki Dam
YPP

29-Jul-2004
29-Jul-2004
27-Jul-2005
29-Jul-2004
27-Jul-2005
30-Jul-2004
27-Jul-2005
3-Aug-2003
31-Jul-2005
29-Jul-2004
27-Jul-2005

ࢆ⾜ࡗ࡚࠾ࡾ㸪ᅇ཰ࡋࡓࢲ࣒ሁ✚≀ࡣࢲ࣒࿘㎶ࡢฎศሙ࡟࠾࠸
࡚ᇙࡵ❧࡚ฎศࡉࢀࡿ㸬ࡋࡓࡀࡗ࡚㸪㧗⃰ᗘ࡟ࣄ⣲ࢆྵࡴᅵ◁ࡀࢲ࣒࿘㎶࡟⵳✚ࡉࢀ࡚࠸ࡿࡢࡀ

Arsenic
content⌧≧࡛࠶ࡿ㸬ࡇࡢሁ✚ฎศሙ࠿ࡽࡢࣄ⣲ࡢ஧ḟⓗ(mg /L)Yu RiverἨᆅᇦ࠿ࡽᇦእ࡬࡜㐠ᦙࡉࢀࡿࣄ⣲ࡢ⥲㔞࡛࠶ࡿ㸬࡞࠾㸪ရᮌࢲ࣒࡛ࡣ୰࿴⏕ᡂ⾲㻞㻌୰࿴ᚋ䛾ἙᕝỈ䛾⁐Ꮡ䝠⣲⃰ᗘ

Sampling locationᕝ࡬ࡢᨺฟཱྀ࡜࡞ࡿ‫‮‬ᕝⓎ㟁ᡤࡢᨺฟỈ୰ࡢࣄ

Flow
rate*

Arsenic
content

Sampling dateሁ✚ࡋ࡚࠸ࡿࡇ࡜ࢆព࿡ࡍࡿ㸬ရᮌࢲ࣒࠿ࡽⓑ◁࡞ᣑᩓ࡟ࡘ࠸࡚ࡣ㸪⎔ቃ㈇ⲴࡢほⅬ࠿ࡽ௒ᚋ༑ศ

ND
ND
ND
ND
ND
ND
ND
ND
ND
ND
ND

࡟᳨ウࡍࡿᚲせࡀ࠶ࡿࡶࡢ࡜⪃࠼ࡽࢀࡿ㸬
4.3 ୰࿴⏕ᡂ≀࡬ࡢࣄ⣲ࡢྲྀࡾ㎸ࡳඛ࡟♧ࡋࡓࡼ࠺࡟㸪ἙᕝỈ࡟⁐Ꮡࡍࡿࣄ⣲ࡣ୰࿴࡟ࡼࡾ⏕ࡌࡿᠱ⃮≀࡟ྲྀࡾ㎸ࡲࢀ࡚࠸ࡿ㸬ࡑࡇ࡛㸪࣓ࣥࣈࣛࣥࣇ࢕ࣝࢱ࡟ࡼࡾᤕ㞟ࡋࡓ୰࿴ᚋࡢ
‫‮‬ᕝ࡞ࡽࡧ࡟ရᮌࢲ࣒ࡢᠱ⃮≀ࡢࣄ⣲⃰ᗘࢆồ

ND: Not detected ( < 0.01 mg /L)ࡵࡓ࡜ࡇࢁ㸪1 wt㸣๓ᚋࡢ㧗࠸ࣄ⣲⃰ᗘࡀᚓࡽࢀ

࡜ࡇࢁ࡛㸪ࡇࡇᩘᖺࡢࣄ⣲⃰ᗘ࡜ࡑࡢ‪ฟ㔞࠿

ࡓ(⾲ 3)㸬ࡉࡽ࡟୰࿴┤ᚋࡢ‫‮‬ᕝࡢἙᗋ࠿ࡽ᥇ྲྀ

ࡽࡍࢀࡤ㸪୓௦㖔※Ἠ࠿ࡽ౪⤥ࡉࢀࡿࣄ⣲ࡣᖺ㛫ࡋࡓ㉥〓Ⰽࡢỿ╔≀ࢆศᯒࡋࡓ࡜ࡇࢁ㸪10 wt%

45 ࢺࣥ࡜ぢ✚ࡶࡽࢀࡿࡢ࡟ᑐࡋ㸪‫‮‬ᕝࡀ㐠ᦙࡍࡿ๓ᚋ࡜ࡁࢃࡵ࡚㧗࠸ࣄ⣲⃰ᗘࢆ♧ࡋ(⾲ 4)㸪୰࿴ࣄ⣲ࡣᖺ㛫 28 ࢺࣥ࡟㐣ࡂ࡞࠸㸬ࡋࡓࡀࡗ࡚㸪ࡑ┤ᚋ࠿ࡽࣄ⣲ࡀ㑅ᢥⓗ࡟୰࿴⏕ᡂ≀࡟྾╔㸪ỿẊࡢᕪ࡜ࡋ࡚ࡢᖺ㛫 10 ᩘࢺࣥࡢࣄ⣲ࡀ⾜᪉୙᫂࡜ࡋ࡚࠸ࡿࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡗࡓ㸬ࡇࡢἙᗋỿẊ≀࡞ࡗ࡚࠸ࡿ㸬ࡇࡢ⾜᪉୙᫂ࡢࣄ⣲ࡢከࡃࡣ㸪వ๫ࡢษ᩿㠃ࢆ EPMA ࡟ࡼࡾᒁᡤศᯒࡋࡓ࡜ࡇࢁ㸪ࡢ୓௦㖔※ἨỈࢆᨺฟụ࡟ᢞධࡍࡿ㝿࡟࿘㎶ᅵࣄ⣲ྵ᭷㔞࡜㕲ྵ᭷㔞࡜ࡢ㛫࡟ࡁࢃࡵ࡚Ⰻ࠸┦ተ࡟ᾐ㏱ࡍࡿ※ἨỈࡸ㸪‫‮‬ᕝࡀὶୗࡍࡿ㐣⛬࡛Ἑ㛫ࡀㄆࡵࡽࢀ(ᅗ 4)㸪Ἑᕝ୰࿴࡟ࡼࡗ࡚⏕ᡂࡍࡿᗋࡸἙᓊ࠿ࡽᅵተ୰࡟ᾐ㏱ࡍࡿἙᕝỈ࡟క࠸ኻỈ㓟໬㕲࡟ࣄ⣲ࡀඹỿࡋ࡚࠸ࡿࡶࡢ࡜⪃࠼ࡽࢀࢃࢀࡓࡶࡢ࡜ᛮࢃࢀࡿ㸬ࡍ࡞ࢃࡕ㸪୓௦㖔※Ἠ࡞

ࡿ㸬XRDࡽࡧ࡟‫‮‬ᕝࡢὶᇦ࡛ࡣ㸪ᅵተ୰࡟ᖺ㛫 10 ࢺࣥ௨࡛࠶ࡾ㸪ࡑࡢ໬Ꮫᙧែࢆ▱ࡿࡇ࡜ࡣ࡛ࡁ࡞࠿ࡗࡓ㸬ୖࡢࣄ⣲ࡀᾐ㏱㸪ᣑᩓࡋ࡚࠸ࡿྍ⬟ᛶࡀ࠶ࡿ㸬ࡋ࠿ࡋ࡞ࡀࡽ‫‮‬ᕝࡢỈ㉁࠿ࡽࡍࢀࡤ㸪ࣄ⣲ࡣࢤ࣮ᐃࡢ⤖ᯝ㸪ࡇࡢἙᗋỿ╔≀ࡣ㠀ᬗ㉁୍᪉㸪୰࿴ᚋࡢἙᕝỈ࡟⁐Ꮡែࡢࣄ⣲ࡀ࡯࡜ࢇࢱ࢖ࢺࡸ࣐࣊ࢱ࢖ࢺ࡞࡝ࡢ㕲㓟໬Ỉ㓟໬≀࡜㸪㕲࡝ㄆࡵࡽࢀ࡞࠸࡜࠸࠺ࡇ࡜ࡣ㸪Ἑᕝ࡟ࡼࡾ㐠ᦙࡉ◲㓟ሷ㖔≀࡛࠶ࡿࢩࣗ࣋ࣝࢺ࣐ࢼ࢖ࢺ࡟ྲྀࡾ㎸ࢀࡿࣄ⣲ࡢ࡯࡜ࢇ࡝ࡀᠱ⃮≀࡜ࡋ࡚ရᮌࢲ࣒࡟

ࡲࢀࡿࡼ࠺࡞ᙧ࡛ỿ╔≀୰࡟Ꮡᅾࡋ࡚࠸ࡿࡶࡢ㻙㻌 㻟㻢㻠㻌㻙

4-6

JAEA-Review 2011-050

࡜᥎ᐹࡉࢀࡿ㸬㕲㓟໬Ỉ㓟໬≀ࡸࢩࣗ࣋ࣝࢺ࣐ࢼ

ᅗ 5 ࡟ࡣ㸪※Ἠ࡞ࡽࡧ࡟‫‮‬ᕝࡢ⁐Ꮡ࢖ࢺࡣ㸪ࣄ⣲ࡢᤕ㞟๣࡜ࡋ࡚ᗈࡃ▱ࡽࢀ࡚࠸ࡿࡶAs(III)/As(V)⃰ᗘࢆ♧ࡋࡓ㸬‪ฟ┤ᚋࡢ※ἨỈ୰ࡢ࡛࠶ࡿ[7,8]㸬

ࡢࣄ⣲ࡣࡑࡢ࡯࡜ࢇ࡝ࡀ As(III)࡛࠶ࡿࡢ࡟ᑐࡋ㸪⾲㻟㻌୰࿴ᚋ䛾Ἑᕝᠱ⃮≀䛾䝠⣲⃰ᗘ㻔஝⇱㔜㔞ᇶ‽㻕୰࿴๓ࡢ‫‮‬ᕝ࡛ࡣ As(III)ࡼࡾࡶ As(V)ࡢ᪉ࡀ༟㉺ࡍࡿࡇ࡜࠿ࡽ㸪※ἨỈࡀࢆ㐠ᦙࡉࢀࡿ㐣⛬࡛ࣄ⣲ࡀ As(III)࠿ࡽ As(V)࡬࡜

YU-A1

29-Jul-2004

1.2

㓟໬ࡉࢀ࡚࠸ࡿࡇ࡜ࡀ♧ࡉࢀࡿ㸬୍᪉㸪୰࿴┤ᚋ

YU-A2

29-Jul-2004

1.2

ࡢ‫‮‬ᕝ࡛ࡣ඲ࣄ⣲⃰ᗘࡀ⣙༙ศ࡜࡞ࡿ࡜࡜ࡶ࡟㸪

SKD

3-Aug-2003

1.6⁐Ꮡࡍࡿࣄ⣲ࡢ࡯࡜ࢇ࡝ࡀ As(III)࡛࠶ࡿࡇ࡜࠿

YPP

29-Jul-2004

0.8

ࡽ㸪As(V)ࡀ㑅ᢥⓗ࡟୰࿴⏕ᡂ≀࡟ྲྀࡾ㎸ࡲࢀ࡚

Sampling location

Yu RiverἨ⾤࡛฼⏝ࡉࢀ㸪Ἑᕝ

Arsenic content
Sampling date
(wt.%)

Shinaki Dam࠸ࡿࡶࡢ࡜ᛮࢃࢀࡿ㸬ࡉࡽ࡟୰࿴ᚋࡢ‫‮‬ᕝࡀࡑࡢୗὶࡢရᮌࢲ࣒࡟ὶධࡍࡿẁ㝵࡟࠾࠸࡚ࡣ㸪඲ࣄ⾲㻠㻌୰࿴┤ᚋ䛾‫‮‬ᕝ䛛䜙᥇ྲྀ䛧䛯Ἑᗋỿ╔≀䛾໬Ꮫ⤌ᡂ⣲⃰ᗘࡣࡉࡽ࡟పୗࡍࡿࡀ㸪As(V)⃰ᗘ࡜࡯ࡰྠ

Content (wt.%)
dark
brown

whitishbrown⛬ᗘ࡛࠶ࡿࡇ࡜࠿ࡽ㸪ὶୗࡍࡿ㐣⛬࡛ As(III)ࡀ

reddish
brown

Na

0.07

0.03

0.02

Mg

0.15

0.11

0.03

Al

1.07

4.93

1.70

Si

15.0

20.3

20.5

P

1.45

1.27

2.02

K

0.12

0.09

0.03

Ca

1.85

0.78

0.20
0.04

As(V)࡟㓟໬ࡉࢀ㸪⏕ࡌࡓ As(V)ࡀ㡰ḟ㸪୰࿴⏕ᡂ≀࡟ྲྀࡾ㎸ࡲࢀ࡚࠸ࡿࡶࡢ࡜⪃࠼ࡽࢀࡿ㸬

Ti

0.21

0.23

Mn

0.04

0.04

0.04

Fe

21.73

28.43

29.62

ᅗ ※ἨỈ࠾ࡼࡧἙᕝỈࡢ $V ,,, ࡜ $V 9 ⃰ᗘ

As

8.8

7.6

9.1

‫※ࡣە‬Ἠ㸪‫ࡣۑ‬ἙᕝỈࢆ♧ࡍ㸬‫ࡣۼ‬୰࿴ᆅⅬ㸬ᅗ୰ࡢ⃰ᗘ⾲グࡣ͆$V ,,, ⃰ᗘ㸭$V 9 ⃰ᗘ͇࡛ PJ/ ༢఩㸬50
y = 1.76x+10.1
r = 0.84

4.5 ᅵተ୰ࡢࣄ⣲⃰ᗘࡢศᕸ40

Fe (wt%)ࣄ⣲⃰ᗘࢆồࡵࡓᅵተࡢ᥇ྲྀ఩⨨ࢆᅗ 6 ࡟♧ࡍ㸬ࡲࡓᚓࡽࢀࡓࣄ⣲⃰ᗘࢆ⾲ 5 ࡟♧ࡍ㸬ࣄ⣲⃰ᗘࡢ30ᆅᇦⓗศᕸࢆぢ࡚ࡳࡿ࡜㸪ⲡὠἨᆅᇦࡢእ⦕㒊࡛ࡣ⃰ᗘࡀపࡃ㸪ሗ࿌ࡉࢀ࡚࠸ࡿᅜෆࡢᆅẆࡸἙ

20ᕝሁ✚≀࡟࠾ࡅࡿࣄ⣲⃰ᗘ(7㹼9 mg/kg)[9,10]࡜
10࡯ࡰྠ➼࡛࠶ࡿࡢ࡟ᑐࡋ㸪ⲡὠἨࡢ୰ᚰ㒊࡟࠾

࠸࡚ࡣ㧗࠸ࣄ⣲⃰ᗘࡀㄆࡵࡽࢀ㸪≉࡟୓௦㖔※Ἠ05

10
As (wt%)15

࿘㎶ࡢᅵተ୰࡟ࡁࢃࡵ࡚㧗࠸⃰ᗘࡀᩓぢࡉࢀࡿ㸬

20ࡋࡓࡀࡗ࡚㸪ⲡὠᅗ ‫‮‬ᕝἙᗋỿ╔≀ࡢ (30$ ࡢᒁᡤศᯒ࡟ࡼࡾᚓࡽࢀࡓ

Ἠᆅᇦ඲య࡟㸪 ἨỈ㉳※ࡢࣄ⣲ࡀᗈࡃᾐ㏱㸪ᣑᩓࡋ࡚࠸ࡿࡶࡢ࡜ぢࡽࢀࡿ㸬୓௦㖔※Ἠ࿘㎶ࡢᅵተ࡟ࡘ࠸࡚ࡼࡾヲ⣽࡟ぢ$V ࡜ )H ࡢ⃰ᗘ┦㛫࡚ࡳࡿ࡜㸪୓௦㖔ࡢ‪ฟཱྀ࿘㎶ࡢᅵተ࡟ࡣࡉ࡯࡝
4.4 ἙᕝỈࡢὶୗ࡟క࠺⁐Ꮡࣄ⣲ࡢ㓟໬㧗࠸ࣄ⣲⃰ᗘࡣㄆࡵࡽࢀࡎ㸪వ๫ࡢ୓௦㖔※ἨỈ

4-6

㻙㻌 㻟㻢㻡㻌㻙

JAEA-Review 2011-050

ࡀ‫‮‬ᕝ࡟ᨺฟࡉࢀࡿᆅⅬࡢ㏆ഐ(Nos. 6 – 8)࡛ࡢࣄ⣲⃰ᗘࡀࡁࢃࡵ࡚㧗࠸㸬‫‮‬ᕝ࡬ࡢ※ἨỈࡢᨺฟ⾲㻡㻌ⲡὠࡣ㸪ᛴᩳ㠃ࡢୗ㒊࡟࠾࠸࡚㸪ᇙタࡉࢀࡓᘬ‫࢖ࣃ‮‬
ࣉࢆ㏻ࡌ࡚┤᥋ⓗ࡟※ἨỈࢆᢞධࡍࡿࡇ࡜࡛࡞
ࡉࢀ࡚࠾ࡾ㸪ࡇࡢᆅⅬࡀ஦ᐇୖࡢ‫‮‬ᕝࡢ㉳Ⅼ࡜࡞ࡗ࡚࠸ࡿ㸬ࡇࡢᨺฟᆅⅬࡢ‫‮‬ᕝἙᓊࡢᅵተ(No. 8)࡛㧗࠸ࣄ⣲⃰ᗘࡀぢ࠸ࡔࡉࢀࡿࡢࡣ㸪᫂ࡽ࠿࡟※ἨỈࡢᾐ㏱࡟క࠸ࣄ⣲ࡀᅵተ୰࡟ྲྀࡾ㎸ࡲࢀ࡚࠸ࡿࡇ࡜ࢆ♧ࡋ࡚࠸ࡿ㸬୍᪉㸪ᨺฟⅬࡢ࠶ࡿᩳ㠃ࡢୖ㒊(No. 6)࡟࠾࠸࡚ࡶ㧗࠸ࣄ⣲⃰ᗘࡀㄆࡵࡽ
ࢀࡿࡀ㸪ࡇࡕࡽࡣᘬ‫ࡢࡽ࠿ࣉ࢖ࣃ‮‬₃Ỉ࡟ࡼࡾ㸪ᅵተ୰࡟※ἨỈࡀᾐ㏱ࡋ࡚࠸ࡿྍ⬟ᛶࡀ㧗࠸㸬Ἠᆅᇦ䛾ᅵተ୰䛾䝠⣲⃰ᗘSampling
location

Sample
No.

1
2

1
2
3A
3B
3C
4
5

Depth
(cm)

As content *(mg/kg)20
15 㼼 11021 㼼 225
37 㼼 113
15
31 㼼 745
36 㼼 5431
17 㼼 45
15
28 㼼 215
170 㼼 26
6
52
87 㼼 2119
36 㼼 6
7A
25
7 㼼 2
7
7B
17
19 㼼 117C
17
33 㼼 48828
130 㼼 30991241 㼼 910101046 㼼 1311
11
10
21 㼼 31212
20
24 㼼 213
13
25
19 㼼 214
14
20
35 㼼 1515
15
22
10 㼼 516
16
20
38 㼼 1
17
17
20
9 㼼 1
18
18
55
8 㼼 1
19
19
45
13 㼼 120
20
53
11 㼼 2* The error twice the standard deviation (±2)of the mean values (n = 3).

㧗࠸ࣄ⣲⃰ᗘࢆ♧ࡋࡓ‫‮‬ᕝ࡟࠾ࡅࡿ※ἨỈᨺ
ฟᆅⅬ࿘㎶ࡢ 2 Ⅼ(Nos. 6, 7)࡟࠾࠸࡚㸪ࡑࡢࣄ⣲⃰ᗘࢆ῝ᗘู࡟ぢ࡚ࡳࡿ࡜㸪ୗᒙࡼࡾୖᒙ࡛ࣄ⣲⃰ᗘࡀ㧗࠸⤖ᯝ࡜࡞ࡗࡓ㸬ᨺฟᆅⅬࡢ‫‮‬ᕝἙᓊࡢᅵተࡢ໬Ꮫ⤌ᡂࡸ㖔≀⤌ᡂ࠿ࡽࡣ㸪᫂ࡽ࠿࡟῝㒊࡛ࡣ㓟ᛶኚ㉁ࡀ㐍⾜ࡋ࡚࠸ࡓ㸬ࡇࡢ㓟ᛶኚ㉁ᒙࡼ
ࡾࡶୖ㒊࡟᭱኱ࣄ⣲⃰ᗘࡀぢࡽࢀࡿࡢ࡛㸪ᙉᗘ࡟㓟ᛶኚ㉁ࡀ㐍⾜ࡋࡓᅵተ࡟ࡣࣄ⣲ࡣಖᣢࡉࢀ࡞
࠸ࡇ࡜ࡀࢃ࠿ࡿ㸬ࡋࡓࡀࡗ࡚㸪୓௦㖔※Ἠࡢᨺฟᅗ ᅵተヨᩱࡢ᥇ྲྀᆅⅬ࡜ヨᩱ␒ྕ D ⲡὠⓑ᰿ⅆᒣᮾ㯄඲ᇦᅗ㸪 E ୓௦㖔※Ἠ࿘㎶ᣑ኱ᅗ㸬‫ࡣۑ‬ᅵተ᥇ྲྀ఩⨨㸪‫※ࡣە‬Ἠ㸬 E ᅗ࡟࠾ࡅࡿ
Ⅼ⥺▮༳ࡣ୓௦㖔※ἨỈࡢᘬ‫⤒‮‬㊰ࢆ♧ࡍ㸬ᆅⅬ࿘㎶࡛ࡣ㸪ᆅ⾲ୗࡢẚ㍑ⓗὸ࠸㒊ศࢆỈᖹ᪉ྥ࡟ᗈࡀࡿࡼ࠺࡟ࣄ⣲ࡀศᕸࡋ࡚࠸ࡿࡶࡢ࡜⪃࠼ࡽࢀࡿ㸬
4.6 ᅵተ୰࡛ࡢࣄ⣲ࡢᙧែ௒ᅇࡢᅵተヨᩱ୰࡛᭱኱ࡢࣄ⣲⃰ᗘࢆ♧ࡋࡓ
No.6 ᆅⅬࡢヨᩱ࡟ᑐࡋ㸪ᅵተศᯒ࡛⏝࠸ࡽࢀࡿ㏲

4-6

㻙㻌 㻟㻢㻢㻌㻙

JAEA-Review 2011-050

ḟ ⁐ ゎ ἲ [11] ࢆ 㐺 ⏝ ࡋ ࡓ 㸬 ㏲ ḟ ⁐ ゎ ἲ ࡛ ࡣ 㸪࡜ࡋ࡚㕲࡜࡜ࡶ࡟◲໬≀ࡢࡼ࠺࡞ᙧែ࡛ᅵተ୰STEP1 ࡟࠾࠸࡚ᙅ㓟ྍ⁐ᛶ࡞ࡽࡧ࡟࢖࢜ࣥ஺᥮

࡟ಖᣢࡉࢀ࡚࠸ࡿࡶࡢ࡜ぢࡽࢀࡿ㸬ࡋ࠿ࡋ࡞ࡀࡽ㸪ែࡢᡂศࢆ㸪STEP2 ࡟࠾࠸࡚㓟໬≀ែ(㑏ඖ⁐ゎࡇࡢࣄ⣲ࡢ㑏ඖ໬ྜ≀ࡀ※ἨỈ࡟ࡼࡿ┤᥋ⓗసᛶ)ࡢᡂศࢆ㸪STEP3 ࡟࠾࠸࡚㑏ඖែ(㓟໬⁐ゎᛶ)⏝࡟ࡼࡗ࡚ᙧᡂࡉࢀࡓࡶࡢ࡞ࡢ࠿㸪ࡑࢀ࡜ࡶ⏕≀࡞ࡽࡧ࡟᭷ᶵ≀ែࡢᡂศࢆ㸪ࡑࢀࡒࢀẁ㝵ⓗ࡟ᢳᏛⓗస⏝࡟ࡼࡗ࡚஧ḟⓗ࡟ᙧᡂࡉࢀࡓࡶࡢ࡞ࡢ

ฟࡋ㸪ᢳฟᾮࡢ໬Ꮫ⤌ᡂ࠿ࡽᅵተ୰࡛ࡢྛᡂศࡢ

࠿ࡣ⌧ẁ㝵࡛ࡣࢃ࠿ࡽ࡞࠸㸬໬Ꮫᙧែࢆ㢮᥎ࡍࡿࡇ࡜ࡀྍ⬟࡛࠶ࡿ㸬⾲ 6 ࡟ࡣ㸳㸬ࡲ࡜ࡵ㏲ḟ⁐ゎࡢ⤖ᯝࢆ♧ࡋࡓ㸬ⲡὠ

⾲6 ㏲ḟ⁐ゎ䛻䜘䜛ᅵተヨᩱ(No.6)䛾ඖ⣲ᢳฟ㔞
Depth

Elementࡍࡿ࡭ࡃ㸪ྠᆅᇦෆࡢ※ἨỈ㸪ἙᕝỈ㸪ᅵተ୰ࡢ

Extracted amount
STEP1
STEP2
STEP3

Al
Fe
Ca
Mg
Ti
Na
K
As

mg/g
mg/g
mg/g
mg/g
mg/g
mg/g
mg/g
Pg/g

0.88
0.024
0.11
0.011
0.0002
0.086
0.15
0.24

5.6
0.90
0.072
0.017
0.005
0.087
0.0014
2.9

4.2
3.4
0.037
0.012
0.053
0.17
0.039
21

Al
Fe
Ca
Mg
5-10 cm
Ti
Na
K
As

mg/g
mg/g
mg/g
mg/g
mg/g
mg/g
mg/g
Pg/g

1.09
0.041
0.10
0.013
0.0007
0.072
0.44
0.42

7.5
0.91
0.051
0.012
0.005
0.067
0.047
3.8

6.4
4.4
0.020
0.008
0.061
0.13
0.090
30

Al
Fe
Ca
Mg
10-15 cm
Ti
Na
K
As

mg/g
mg/g
mg/g
mg/g
mg/g
mg/g
mg/g
Pg/g

0.94
0.029
0.12
0.015
0.0004
0.099
0.44
0.25

6.4
0.93
0.066
0.015
0.005
0.10
0.059
3.6

4.7
4.0
0.029
0.011
0.067
0.22
0.12
25

0-5 cmἨᆅᇦ࡟࠾ࡅࡿࣄ⣲ࡢືែࢆ᫂ࡽ࠿࡟

ࣄ⣲⃰ᗘࢆ✀ࠎࡢᡭἲ࡛ồࡵࡓ㸬ࡇࡢ⤖ᯝ㸪௨ୗࡢࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡗࡓ㸬(1) ⲡὠ

Ἠᆅᇦࡢ※ἨỈ࡞ࡽࡧ࡟ἙᕝỈࡢࣄ⣲⃰ᗘ࡟ᇶ࡙ࡃ࣐ࢫࣂࣛࣥࢫィ⟬ࡢ⤖ᯝ㸪ᙜヱᆅᇦ࡟࠾࠸࡚୓௦㖔※Ἠࡀ᭱኱ࡢࣄ⣲౪⤥※࡛࠶ࡾ㸪ᖺ㛫⣙ 45 ࢺࣥࡢࣄ⣲ࢆᨺฟࡋ࡚࠸ࡿ㸬ࡲࡓ㸪୓௦㖔※ἨỈࡀὶධࡍࡿ‫‮‬ᕝ࡛ࡣ㸪ᖺ㛫⣙ 28 ࢺࣥࡢࣄ⣲ࡀ㐠ᦙࡉࢀ࡚࠸ࡿ㸬※Ἠ࠿ࡽࡢࣄ⣲౪⤥㔞࡜Ἑᕝ࡟ࡼࡿࣄ⣲㐠ᦙ㔞ࡢᕪ࠿ࡽࡍࢀࡤ㸪ᖺ㛫 10 ࢺࣥ௨ୖࡢࣄ⣲ࡀ㸪ᙜヱᆅᇦࡢᅵተ୰࡟ᾐ㏱㸪ᣑᩓࡋ࡚࠸ࡿ࡜ぢࡽࢀࡿ㸬(2) ἙᕝỈ୰ࡢࣄ⣲ࡣ㸪ᙜヱᆅᇦࡢ㓟ᛶἙᕝ୰࿴
஦ᴗ࡟ࡼࡾ⏕ࡌࡿ୰࿴⏕ᡂ≀࡟ᤕ㞟ࡉࢀ㸪ࡑࡢ኱༙ࡀရᮌࢲ࣒࡟⵳✚ࡋ࡚࠸ࡿ㸬ရᮌࢲ࣒࡟ࡣᖺ㛫⣙ 25 ࢺࣥࡢࣄ⣲ࡀ⵳✚ࡋ㸪ᖺ㛫 3ࢺࣥࡢࣄ⣲ࡀᆅᇦእ࡟ᠱ⃮≀࡜ࡋ࡚㐠ᦙࡉࢀ࡚࠸ࡿ࡜ぢ✚ࡶࡽࢀࡓ㸬(3) Ἑᕝ୰࿴஦ᴗ࡛ࡣ㸪As(V)ࡀ㑅ᢥⓗ࡟୰࿴⏕ᡂ≀࡟ྲྀࡾ㎸ࡲࢀ㸪As(III)ࡣἙᕝࡢὶୗ࡟క࠸
ᚎࠎ࡟ As(V)࡟㓟໬ࡉࢀࡿࡇ࡜࡛㸪㡰ḟ㸪୰

⾲ 6 ࢆぢ࡚ࡢ㏻ࡾ㸪ࣄ⣲ࡣ STEP3 ࡟࠾࠸࡚ᢳ

࿴⏕ᡂ≀࡬࡜྾╔㝖ཤࡉࢀࡿ㸬ฟࡉࢀࡿ๭ྜࡀ᭱ࡶ㧗ࡃ㸪ᅵተ୰࡛ࡣࡑࡢከࡃࡀ
㑏ඖែ࡜ࡋ࡚Ꮡᅾࡋ࡚࠸ࡿࡇ࡜ࢆ♧ࡋ࡚࠸ࡿ㸬ࣄ(4) ୓௦㖔※Ἠࡢ࿘㎶ࡢᅵተ୰࡟ࡣ㸪※ἨỈࡢᾐ⣲௨እࡢᡂศ࡛ࡣ㸪㕲ࡀࣄ⣲࡜㢮ఝࡢᢳฟᣲືࢆ

㏱ࡢ⤖ᯝ࡜ࡋ࡚㧗࠸ࣄ⣲⃰ᗘࡀぢ࠸ࡔࡉࢀࡿ㸬♧ࡋ㸪STEP3 ࡛ࡢᢳฟࡀ༟㉺ࡋ࡚࠸ࡿ㸬ࡇࡢࡇᅵተ୰ࡢࣄ⣲ࡣ As(III)࡜ࡋ࡚㕲࡜࡜ࡶ࡟ᅛ

࡜ࡣ㸪ᅵተ୰࡛ࣄ⣲ࡀ㕲࡜࡜ࡶ࡟㑏ඖែࡢ໬ྜ≀ᐃࡉࢀ࡚࠸ࡿ࡜ぢࡽࢀࡿ㸬ࢆᵓᡂࡋ࡚࠸ࡿࡇ࡜ࢆ♧၀ࡋ㸪ᑡ࡞ࡃ࡜ࡶࣄ⣲ࡀ㓟໬ែ࡛࠶ࡿ㕲㓟໬≀➼࡟྾╔ࡋ࡚࠸ࡿࡢ࡛ࡣ

ཧ⪃ᩥ⊩࡞࠸ࡇ࡜ࢆព࿡ࡍࡿ㸬࠾ࡑࡽࡃࡣ㸪ࣄ⣲ࡣ As(III)[1] బ⸨ẚዉᏊ㸪▼ᒣ኱୕㸪Ỉ⏣ᩄኵ㸪ୡⰋ⪔୍㻙㻌 㻟㻢㻣㻌㻙

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JAEA-Review 2011-050

㑻㸪⛅⏣┴⋢ᕝἨࡢ኱ᄇ࡜‫‮‬ᕝࡢ

Geosyst.,ἨỈ࡜ỿẊ≀ࡢ≉ᚩ㸬NMCC ඹྠ฼⏝◊✲ᡂᯝሗᩥ㞟㸪
12㸪205-211㸪2004㸬

1,

doi:10.1029/2000GC000083,

2000.
[10] ௒஭Ⓩ㸪ᑎᓥ⁠㸪ኴ⏣඘ᜏ㸪ᚚᏊᰘ㸦Ặᐙ㸧[2] ᮌᕝ⏣႐୍㸪኱஭㝯ኵ㸪ᕝ஭ᬛ㸪㛗㇂ᕝ₶㸪┿⃈㸪ᒸ஭㈗ྖ㸪❧ⰼዲᏊ㸪ᐩᶔⱱᏊ㸪ᯇஂᖾᑠᆏ⨾⣖Ꮚ㸪㔠⏣ဴே㸪᪩ὠᓅᏹ㸪బ㔝῟Ꮚ㸪ᩗ㸪㔠஭㇏㸪ୖᒸ᫭㸪㇂ཱྀᨻ☒㸪᪥ᮏࡢᆅ⌫໬ஂ㔝ྜྷ㑻㸪す㔝๛ᘯ㸪ⲡὠⓑ᰿ᒣ࿘㎶Ꮫᅗ㸬ᆅ㉁ࢽ࣮ࣗࢫ㸪604㸪30-36㸪2004㸬Ἠࡢᚤ㔞ඖ⣲⁐Ꮡ⃰ᗘࡢ⤒ᖺኚ໬࡜ࡑࡢᆅ⌫໬Ꮫⓗゎ[11] G. Rauret, J. F. López-Sánchez, A.

㔘㸬ᖹᡂ 16 ᖺᗘཎ◊᪋タ฼⏝ඹྠ◊✲ᡂᯝሗ

Sahuquillo, R. rubio, C. Davidson, A. Ure, P.

࿌᭩㸪59-65㸪2005㸬

Quevauviller, Improvement of the BCR three[3] ᑠᆏ୔ண㸪ᑠᆏ▱Ꮚ㸪ᖹᯘ㡰୍㸪኱஭㝯ኵ㸪

step sequential extraction procedure prior to኱ሙṊ㸪㔝ୖ೺἞㸪ᮌᕝ⏣႐୍㸪㣕⏣඾Ꮚ㸪୓the certification of new sediment and soil

௦㖔※Ἠࡢ‪ฟ࡟క࠺ⲡὠ

reference materials. J. Environ. Monit., 1,໬࡟ࡘ࠸࡚㸬

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Ἠ⛉Ꮫ㸪47㸪166-178㸪1998㸬

57-61, 1999.

[4] Y. C. Sun, J. Y. Yang, Simultaneous
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ᡂᯝࡢබ⾲(IV,VI), and antimony (III,V) in natural waterᏛ⾡ㄽᩥ

by coprecipitation and neutron activationzᮌᕝ⏣႐୍㸪ᕝ஭ᬛ㸪኱஭㝯ኵ (2006) ⲡὠanalysis. Anal. Chim. Acta, 395, 293-300,

Ἠ୺せ※Ἠ࡟࠾ࡅࡿ⁐Ꮡࣄ⣲⃰ᗘ⤒ᖺኚ໬ ࡜ ࣄ ⣲ ㈇ Ⲵ 㔞 ࡢ ぢ ✚ 㸬 ᆅ ⌫ ໬ Ꮫ 㸪 40 㸪

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Kikawada, Y., Fuji, H, Ohono, Y, Oi, T.

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the orogenic Japan Arc. Geochem. Geophys.

⣖せ➼㻙㻌 㻟㻢㻤㻌㻙

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JAEA-Review 2011-050

zᮌᕝ⏣႐୍㸪ᮏከ↷ᖾ㸪኱஭㝯ኵ (2006) ⲡᑕ໬ศᯒ࡟ࡼࡿ As ౯ᩘูᐃ㔞ἲ㸪2006 ᖺᗘὠ᪥ᮏᆅ⌫໬Ꮫ఍ㅮ₇せ᪨㞟㸪p.3㸬

Ἠ୺せ※Ἠ࠾ࡼࡧ࿘㎶Ἑᕝ࡟ࡼࡿࣄ⣲㈇Ⲵ㔞ࡢぢ✚㸬 Ṋⶶᕤᴗ኱ᏛཎᏊຊ◊✲ᡤzᡤሗ㸪32㸪6-13㸬zబ㔝῟Ꮚ㸪ᮌᕝ⏣႐୍㸪኱஭㝯ኵ (2007) ⲡὠⓑ᰿ⅆᒣࡢⅆᒣάື࡟㐃ືࡋࡓ୓ᗙ

ᮌᕝ⏣႐୍ (2006) ⅆᒣᛶἨ࡟ぢࡿ⁐Ꮡࣄ

୺せ※Ἠࡢ⁐Ꮡࣄ⣲⃰ᗘ⤒ᖺኚ໬㸬᪥ᮏᆅ⌫⣲⃰ᗘࡢ⤒ᖺኚ໬࡜⎔ቃၥ㢟㸬ᆅୗỈᢏ⾡㸪ᝨᫍ⛉Ꮫ㐃ྜ 2007 ᖺ኱఍ (2007 ᖺ 5 ᭶ 23

48 (12)㸪1-9㸬᪥㸪ᖥᙇ࣓ࢵࢭ)Ꮫ఍Ⓨ⾲z

Kikawada, Y., Kawai, S., Oi, T. (2007)
Effect of Acidic River Water Neutralization
on Mobility of Arsenic in Kusatsu-Shirane
Volcano Area, Gunma, Japan. Cities on
Volcano 5 (COV5) [Shimabara, Japan],
13-O-12.

z

Kikawada, Y., Fuji, H., Ohno, Y., Oi, T.
(2007) Mobility of arsenic in hot springwater accompanying penetration of water
into ground. 12th International ConferenceonModernTrendson

ActivationofAnalysis (MTAA-12) [Hachioji, Japan],
A087.
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Kikawada, Y., Kawai, S., Shimada, K., Oi,
T. (2006) Origin and fate of dissolved
arsenic in acidic rivers in the Kusatsu hot
spring area, Gunma, Japan. 16th Annual
V.M. Goldschmidt Conference [Melbourne,
Australia], Geochim. Cosmochim. Acta, 70,
Suppl. 1, p.15.

zబ㔝῟Ꮚ㸪ᕝ஭ᬛ㸪ᮌᕝ⏣႐୍㸪኱஭㝯ኵ
(2005) ⲡ ὠ ⓑ ᰿ ᒣ す 㯄 㝣 Ỉ ࡢ ࣄ ⣲ ⃰ ᗘ 㸪
2005 ᖺᗘ᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ㅮ₇せ᪨㞟㸪
p.156㸬zᮌᕝ⏣႐୍㸪ᕝ஭ᬛ㸪బ㔝῟Ꮚ㸪኱஭㝯ኵ
(2005) ⩌㤿┴ⲡὠⓑ᰿ᒣᮾ㯄※Ἠ࡞ࡽࡧ࡟
Ἑᕝ࡟࠾ࡅࡿࣄ⣲ࡢ≀㉁཰ᨭ㸪2005 ᖺᗘ᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ㅮ₇せ᪨㞟㸪p.283㸬zἨబ㔝῟Ꮚ㸪ᕝ஭ᬛ㸪ᮌᕝ⏣႐୍㸪኱஭㝯ኵ
(2006) Pb(PDC)2 ඹỿἲࢆ฼⏝ࡋࡓ୰ᛶᏊᨺ㻙㻌 㻟㻢㻥㻌㻙

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JAEA-Review 2011-050

4-7⏿ᆅ࡟࠾ࡅࡿ᭷ᶵᛶᗫᲠ≀࡟⏤᮶ࡍࡿᅵተᨵⰋ㈨ᮦࡢ᪋⏝ࡀྛ✀ඖ⣲ࡢᅵተ⵳✚࡜స≀྾཰࡟ཬࡰࡍᙳ㡪$FFXPXODWLRQRIHOHPHQWVLQDQDUDEOHILHOGZLWKVRLODPHQGPHQWV RUJDQLFXQXVHGUHVRXUFHV DQGLWVXSWDNHE\FXOWLYDWHGFURS༓ⴥ኱Ꮫ㸸㕥ᮌᘯ⾜࣭⇃㇂ ᏹᮾி኱Ꮫ㸸㔝ᕝ᠇ኵ
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ᨵⰋ㈨ᮦ࡛࠶ࡿୗỈởἾࢥ࣏ࣥࢫࢺࢆᨺᑕ໬ศᯒࡋ
ࡓ⤖ᯝ㸪=Q㸪$J㸪/D ➼ከᩘࡢ㔜㔠ᒓࡀྵࡲࢀ࡚࠸ࡿ
ࡇ࡜ࡀ᫂ࡽ࠿࡜࡞ࡗࡓࠋࡲࡓ㸪ࡑࡢࡼ࠺࡞ୗỈởἾࢥ࣏ࣥࢫࢺࢆ᪋⏝ࡋࡓᅡሙࡢᅵተ࡟࠾࠸࡚ $J ࡀ⵳✚ࡋ࡚࠸ࡿࡇ࡜ࡶ᫂ࡽ࠿࡟࡞ࡗࡓࠋࡋ࠿ࡋ㸪ୗỈởἾࢥ࣏ࣥࢫࢺࡢᢞධ㔞࠿ࡽ᥎ᐃࡋࡓᅡሙࡢᅵተࡢ
$J ྵ᭷⋡㸦ศᩓࡍࡿᅵᒙࢆ FP ࡜௬ᐃ㸧ࡣᐇ ್ࡼࡾపࡃ࡞ࡿࡓࡵ㸪ࡑࡢཎᅉࢆㄪᰝࡍࡿᚲせࡀ࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋ
ࡇࡢࡓࡵ㸪ᖹᡂ  ᖺࠥ ᖺᗘࡢཎ◊᪋タ฼⏝ඹྠ◊✲࡟࠾࠸࡚ࡣ㸪ูᖺᗘ࡟᥇ྲྀࡋࡓᅵተヨᩱࢆ⏝࠸࡚ྛඖ⣲ࡢᅵተྵ᭷⋡࡟ࡘ࠸࡚෌ホ౯ࢆ⾜ࡗࡓࠋࡲࡓ㸪ᅵተᨵⰋ㈨ᮦ࡛࠶ࡿୗỈởἾࢥ࣏ࣥࢫࢺࡢ᪋
⏝ୗ࡛᱂ᇵࡋࡓస≀࡟ࡘ࠸࡚㔜㔠ᒓࡸࡑࡢ௚ࡢᵝࠎ࡞ඖ⣲ࡢྵ᭷⋡ࢆㄪ࡭㸪໬Ꮫ⫧ᩱࡢࡳࢆ᪋⏝ࡋࡓሙྜ࡜ẚ㍑ࡋࡓࠋࡑࡢ⤖ᯝ࡟ࡘ࠸࡚ሗ࿌ࡍࡿࠋ
㸦2㸧ヨᩱ࠾ࡼࡧ᪉ἲ ヨ㦂༊ࡢᴫせ༓ⴥ኱ᏛᅬⱁᏛ㒊ෆࡢᅡሙ࡟ࢺࣞࣥࢳ㸦㛗ࡉ P㸪ᖜ P㸪῝ࡉ FP㸧ࢆ᥀ࡾ㸪 ᖺ  ᭶࡟〓Ⰽ᳃ᯘᅵࢆ඘ሸࡋࡓࠋ〓Ⰽ᳃ᯘᅵࡣ༓ⴥ┴ᬮᆅᅬⱁ◊✲ᡤෆࡢ⏿ࡼࡾ᥇ྲྀࡋࡓࠋヨ㦂༊ࡣ໬Ꮫ⫧ᩱ༊࡜࢜࢞ࢡ
ࢬởἾࢥ࣏ࣥࢫࢺ༊㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊ࡢ
 ༊ࢆタ⨨ࡋࡓࠋ໬Ꮫ⫧ᩱ༊ࡣ $ ♫〇ࡢ໬Ꮫ⫧ᩱ㸦1㸸32 㸸.2 㸧ࢆ  స࠶ࡓࡾ WKD ࡲࡓࡣ WKD᪋⏝ࡋࡓࠋ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࡟ࡣ % ᕷ࡟࠾࠸࡚࢜࢞ࢡࢬ࡜ୗỈởἾࢆΰྜࡋሁ⫧໬ࡋࡓ࢜࢞ࢡ
ࢬởἾࢥ࣏ࣥࢫࢺ࡜໬Ꮫ⫧ᩱ༊࡜ྠ㔞ࡢ໬Ꮫ⫧ᩱࢆ᪋⏝ࡋࡓࠋ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊࡟ࡣ㸪& ᕷ࡟࠾࠸࡚࣑ࣔ࢞ࣛ࡜ୗỈởἾࢆΰྜࡋሁ⫧໬ࡋࡓ࣑ࣔ
࢞ࣛởἾࢥ࣏ࣥࢫࢺ࡜໬Ꮫ⫧ᩱ༊࡜ྠ㔞ࡢ໬Ꮫ⫧ᩱࢆ᪋⏝ࡋࡓࠋ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ࡜࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࡣࡑࢀࡒࢀ஝≀࡜ࡋ࡚ึᅇࡢࡳ WKD㸪௨㝆ࡣྛసࡈ࡜࡟ WKD ᪋⏝ࡋࡓࠋヨ㦂ࡣ ᖺ  ᭶࡟㛤ጞࡋ  ᖺ  ᭶ࡲ࡛ࡢ  ᖺ㛫࡟ࢥ࣏ࣥࢫࢺࡣྜィ  ᅇ᪋⏝ࡋࡓࠋࡑࡢ᪋⏝≧ἣ࡜᱂ᇵస≀࡟ࡘ࠸࡚ࡣ⾲  ࡟♧ࡋࡓࠋ ᅵተヨᩱ࠾ࡼࡧస≀ヨᩱࡢㄪᩚ
ᅵተヨᩱࡣ  ᖺ࠾ࡼࡧ  ᖺࡢ  ᭶࡟໬Ꮫ⫧ᩱ㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝๓࡟㸪ྛヨ㦂༊࠿ࡽࣛࣥࢲ࣒࡟  ⟠ᡤࢆ㑅ࡧ㸪ࡑࢀࡒࢀࡢ⾲ᒙᅵ㸦ࠥFP㸧ࢆ᥇ྲྀࡋࡓࠋ
᥇ྲྀࡋࡓᅵተࡣ஝⇱ᚋ⢊○ࡋ PP ࡢ⠠ࢆ㏻㐣ࡉࡏ࡚ศᯒ࡟౪ヨࡋࡓࠋ᱂ᇵస≀ࡢศᯒࡣ  ᖺ  ᭶࡟᥇ྲྀࡋࡓ࢚ࣥࣂࢡ࡜  ᖺ  ᭶࡟᥇ྲྀࡋࡓࢽࣥࢪ
ࣥ࡟ࡘ࠸࡚⾜ࡗࡓࠋ࢚ࣥࣂࢡ࡜ࢽࣥࢪࣥࡣ᥇ྲྀᚋ㸪⵨␃Ỉࢆ⏝࠸࡚Ὑίࡋᅵተ⢏Ꮚ➼ࢆ㝖ཤࡋࡓࠋỈὙᚋ㸪࢚ࣥࣂࢡ࠿ࡽࡣ✑㸪ࢽࣥࢪࣥ࠿ࡽࡣ୺᰿ࡢ⓶ࡸⴥ᯶ᇶ㒊࡞࡝ࡢ㠀ྍ㣗㒊㸦௨ୗ⓶࡜⾲グ㸧㸪⓶ࢆ㝖࠸ࡓ୺᰿㸦௨ୗྍ㣗㒊࡜⾲グ㸧ࢆศ㞳ࡋ㸪Υ࡛ ᫬㛫஝⇱ࡋࡓࠋ஝⇱ᚋ㸪ྛ㒊ศࢆ⢊○ࡋᨺᑕ໬ศᯒ
⏝ࡢヨᩱ࡜ࡋࡓࠋ ୰ᛶᏊᨺᑕ໬ศᯒྛ ヨ ᩱ ࡜ ᶆ ‽ ヨ ᩱ 㸦 1DWLRQDO ,QVWLWXWH RI
6WDQGDUGVDQG7HFKQRORJ\ࡢ 3HDFK/HDYHV650㸪&KLQD1DWLRQDO$QDO\VLV&HQWHUIRU,URQDQG6WHHOࡢ 6WUHDP6HGLPHQW1&6'&㸧ࡢ ࠥPJ ࢆ⛗㔞ࡋ㸪࣏࢚ࣜࢳࣞࣥ〇ࡢᑠ⿄࡟ᑒධࡋࡓࠋࡇࡢᑠ⿄ࡣࡉࡽ࡟ูࡢᑠ⿄࡟ᑒධࡋ஧㔜࡟ࡋࡓࠋ஧㔜໬ࡋࡓᑠ⿄ࡣ↷ᑕ⏝ࡢ࢟ࣕࣉࢭࣝ࡟඘ሸࡋࡓᚋ㸪᪥ᮏཎᏊ ຊ ◊ ✲ ᡤ ᮾ ᾏ ◊ ✲ ᡤ ࡢ ཎ Ꮚ ⅔ -55 ࡲ ࡓ ࡣ-550 ࡟࠾࠸࡚ᨺᑕ໬ࡋࡓࠋᨺᑕ໬ศᯒ࡛ࡣᶆ‽ヨᩱ࠿ࡽ᳨ฟࡉࢀࡓ㸪1D㸪0J㸪&O㸪.㸪&D㸪6F㸪&U㸪0Q㸪
)H㸪&R㸪=Q㸪$V㸪%U㸪5E㸪6U㸪=U㸪$J㸪6E㸪&V㸪%D㸪
/D㸪&H㸪6P㸪(X㸪<E㸪/X㸪7D㸪7K㸪8 ࡢ  ඖ⣲ࢆᐃ㔞ࡢᑐ㇟࡜ࡋࡓࠋヨᩱࡢ↷ᑕ᮲௳࡜ ᐃ᰾✀ࢆ⾲ ࡟♧ࡋࡓࠋ ᐃࡣࢤ࣐ࣝࢽ࣒༙࢘ᑟయ᳨ฟჾࢆ⏝࠸

JRR-3M (PN-1); JRR-4 (Ẽ㏦⟶, T ࣃ࢖ࣉ A), ୰ᛶᏊ฼⏝ศᯒ࣭ᨺᑕ໬ศᯒ㻙㻌 㻟㻣㻜㻌㻙

JAEA-Review 2011-050

࡚⾜࠸㸪Ț⥺࢚ࢿࣝࢠ࣮࡜༙ῶᮇࢆᇶ࡟ᨺᑕ໬ࡉࢀ
ࡓ᰾✀ࡢྠᐃࢆ⾜ࡗࡓࠋࡑࡋ࡚㸪ྛヨᩱ୰ࡢᨺᑕ໬
ࡉࢀࡓ᰾✀ࡢᨺᑕ⬟ࢆᶆ‽ヨᩱ୰ࡢᨺᑕ໬ࡉࢀࡓ᰾
✀ࡢᨺᑕ⬟࡜ẚ㍑ࡋ࡚ᐃ㔞ࢆ⾜ࡗࡓࠋ㸧⤫ィฎ⌮⤫ィゎᯒࢯࣇࢺ 6WDWFHO ࢆ⏝࠸࡚㸪ᅵተ࡜᱂ᇵస≀ࡢࢹ࣮ࢱࡢศᩓศᯒ࡜ከ㔜᳨ᐃ
㸦%RQIHUURQL'XQQ ἲ㸧ࢆ⾜ࡗࡓࠋ㸦3㸧⤖ᯝ࠾ࡼࡧ⪃ᐹ ୗỈởἾࢥ࣏ࣥࢫࢺ࡜໬Ꮫ⫧ᩱ୰ࡢඖ⣲࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ࠾ࡼࡧ໬Ꮫ⫧ᩱࡢศᯒ⤖ᯝࢆ⾲  ࡟♧ࡋࡓࠋ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ࡜࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ࠿ࡽࡣ ᐃࡢᑐ㇟࡜ࡋࡓ  ඖ⣲㸪໬Ꮫ⫧ᩱ࠿ࡽࡣ $Jࢆ㝖࠸ࡓ  ඖ⣲ࡀ᳨ฟࡉࢀࡓࠋ
ࡇࢀࡽࡢඖ⣲ࡢ୰࡛ࡣ =Q ࡟ࡘ࠸࡚㸪ᅵተ࡟⵳✚ࡋࡸࡍ࠸㔜㔠ᒓ࡜ࡋ࡚つไ್ࡀ♧ࡉࢀ࡚࠾ࡾ㸪ᖺ࡟ᨵṇࡉࢀࡓ⫧ᩱྲྀ⥾ἲ࡟࠾࠸࡚ࡣ PJNJ ௨ୖྵࡴሙྜ࡟⾲♧ࡢ⩏ົ௜ࡅࡀ࡞ࡉࢀ࡚࠸ࡿࠋ࢜࢞
ࢡࢬởἾࢥ࣏ࣥࢫࢺ࡜࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࡢ
=Q ྵ᭷⋡ࡣ⣙ PJNJ ࡛࠶ࡾ㸪໬Ꮫ⫧ᩱࡼࡾࡶ⣙㸵ಸ㧗࠸್ࢆ♧ࡋࡓࠋ=Q ࡢࡼ࠺࡟໬Ꮫ⫧ᩱ࡜ẚ࡭࡚㸵ಸ௨ୖ㧗࠸ྵ᭷⋡ࢆ♧ࡋࡓඖ⣲࡟ࡣ㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ࡟࠾࠸࡚ 0Q㸪)H㸪$J㸪%D㸪/D㸪&H ࡀ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ࡟࠾࠸࡚ 0Q㸪$J㸪%D ࡀ࠶ࡗࡓࠋࡇࢀࡽࡢඖ⣲࡟ࡘ࠸࡚ࡣ㸪㛗ᮇ࡟ࢃࡓࡿ᪋⏝࡛ࡣ =Q ྠᵝ࡟ᅵተ࡬ࡢ⵳✚࡟ࡘ࠸࡚ៅ㔜࡟᳨ウࡍࡿ
ᚲせࡀ࠶ࡿ࡜ᛮࢃࢀࡿࠋ ᅵተ୰ࡢඖ⣲ᖹᡂ  ᖺࠥ ᖺᗘࡢཎ◊᪋タ฼⏝ඹྠ◊✲࡟࠾࠸࡚  ᖺ࡟᥇ྲྀࡉࢀࡓᅵተ࡟࠾࠸࡚ࡣ $J ࡀ᳨ฟࡉࢀࡓࡀ㸪 ᐃ࡟⏝࠸ࡓ P$J ࡟ࡘ࠸࡚෭༷ᮇ㛫࡜ ᐃ᫬㛫ࢆ༑ศ࡟ྲྀࡾ NH9 ࡢ࣐࢞ࣥ⥺࡟ࡘ࠸࡚༙ῶᮇࢆ᳨ドࡍࡿ࡜ඹ࡟ NH9㸪NH9㸪NH9㸪NH9 ࡢ࣐࢞ࣥ⥺ࡢᏑᅾ࡟ࡘ࠸࡚ࡶ᳨ドࡋࡓ⤖ᯝ㸪ᅵተヨᩱ࠿ࡽࡣ $J ࡣ᳨ฟࡉࢀ࡚࠸࡞࠸࡜⤖ㄽࡋࡓࠋࡇࡢࡓࡵ㸪 ᖺ࠾ࡼࡧ  ᖺ࡟᥇ྲྀࡋࡓ࢜࢞ࢡ
ࢬởἾࢥ࣏ࣥࢫࢺ༊㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊㸪໬Ꮫ⫧ᩱ༊ࡢᅵተ࠿ࡽࡣ $J ࢆ㝖࠸ࡓ  ඖ⣲ࡀ᳨ฟࡉࢀࡓ㸦⾲ 㸧ࠋ ᖺ࡟᥇ྲྀࡋࡓᅵተ࡛ࡣ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊ࡢ 5E ࡢྵ᭷⋡ࡀ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊
ࡼࡾࡶ᭷ព࡟㧗ࡃ࡞ࡗࡓࡀ㸪୧ởἾࢥ࣏ࣥࢫࢺ༊࡜
ࡶ໬Ꮫ⫧ᩱ༊࡜ࡣ 5E ࡢྵ᭷⋡࡟᭷ព࡞㐪࠸ࡣㄆࡵࡽࢀ࡞࠿ࡗࡓࠋࡲࡓ௚ࡢඖ⣲ࡢྵ᭷⋡࡟ࡣ  ࡘࡢヨ㦂༊ࡢᅵተ㛫࡛᭷ពᕪࡣㄆࡵࡽࢀ࡞࠿ࡗࡓࠋ୍᪉  ᖺ࡟᥇ྲྀࡋࡓᅵተ࡛ࡣ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࡟࠾࠸࡚ =Q㸪6E㸪%D㸪/D㸪&H㸪ࡢྵ᭷⋡ࡀ໬Ꮫ⫧ᩱ༊ࡼࡾࡶ᭷ព࡟㧗ࡃ࡞ࡾ㸪/D ࡜ &H ࡢྵ᭷⋡࡟ࡘ࠸࡚ࡣ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊࡜ࡶ᭷ព
ᕪࡀㄆࡵࡽࢀࡓࠋ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊࡟࠾࠸
࡚ࡣ =Q ࡜ $V ࡢྵ᭷⋡ࡀ໬Ꮫ⫧ᩱ༊ࡸ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊ࡼࡾࡶ᭷ព࡟㧗ࡃ࡞ࡗࡓࠋ
໬Ꮫ⫧ᩱ༊࡜᭷ពᕪࡀㄆࡵࡽࢀࡓởἾࢥ࣏ࣥࢫ
ࢺ༊ࡢඖ⣲࡟ࡘ࠸࡚㸪ởἾࢥ࣏ࣥࢫࢺ༊࡜໬Ꮫ⫧ᩱ༊࡜ࡢᕪࢆඖ⣲ࡢቑຍศ㸦ᐇ ್㸧࡜ࡋ࡚⌮ㄽ್㸦ᖺ㛫ࡢୗỈởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝࡟కࡗ࡚ᢞධࡉࢀ
ࡓඖ⣲ࡀᅵᒙ FP ࡲ࡛࡟ศᩓࡋࡓሙྜࡢ໬Ꮫ⫧ᩱ༊࡜ࡢᕪ㸧࡜ẚ㍑ࡋࡓሙྜ㸦⾲ 㸧࡜ẚ㍑ࡋࡓሙྜ㸪ᐇ ್ࡢ =Q㸪$V㸪6E㸪%D㸪/D㸪&H ࡢྵ᭷⋡ࡢቑຍศࡣ⌮ㄽ್ࡢ 㸣㸪㸣㸪㸣㸪㸣㸪㸣㸪㸣࡟┦ᙜࡋࡓࠋࡇࡢࡓࡵ㸪ࡇࢀࡽࡢඖ⣲࡟ࡘ࠸࡚ࡣᢞ
ධࡉࢀࡓඖ⣲㔞ࡢ 㸣௨ୖࡀᅵᒙ FP ࡲ࡛࡟Ꮡᅾ
ࡍࡿ࡜⪃࠼ࡽࢀࡓࠋࡋ࠿ࡋ㸪ࡇࢀࡽࡢඖ⣲ࢆ ᖺ࡜  ᖺࡢྵ᭷⋡࡛ẚ㍑ࡍࡿ࡜㸪=Q ࡢࡼ࠺࡟ᢞ
ධ㔞࡜ࡋ࡚ࡣ  ᖺࡢ᪉ࡀከ࠸࡟ࡶ࠿࠿ࢃࡽࡎ
 ᖺࡢ᪉ࡀ㧗࠸ഴྥࢆ♧ࡋ࡚࠸ࡿሙྜࡶ࠶ࡿࠋࡇ
ࡢࡼ࠺࡞ඖ⣲ྵ᭷⋡ࡢᖺḟኚືࡣస௜ࡅ᮲௳➼ࡢᙳ㡪ࡀ࠶ࡿࡢ࠿ࡶࡋࢀ࡞࠸ࠋࡇࡢࡓࡵ㸪ᅵተ࡟࠾ࡅࡿ
ඖ⣲ࡢ⵳✚ࢆṇ☜࡟ᢕᥱࡍࡿࡓࡵ࡟ࡣከᖺᗘ࡟ࢃࡓ
ࡿᖺḟኚື࡟ࡘ࠸࡚ࢹ࣮ࢱࢆ㞟ࡵࡿᚲせࡀ࠶ࡿࠋ
ᮏ◊✲ࡢ⤖ᯝ࠿ࡽ㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺࡸ
࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࢆ〓Ⰽ᳃ᯘᅵ࡟  ᖺ㛫ᢞධࡋࡓ㝈ࡾ࡟࠾࠸࡚ࡣ㸪=Q㸪$V㸪6E㸪%D㸪/D㸪&H ࡣᅵተ࡟⵳✚ࡋࡸࡍ࠸ᛶ㉁ࡀ࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋࡲࡓୗ
ỈởἾࢥ࣏ࣥࢫࢺ࡜໬Ꮫ⫧ᩱ୰ࡢඖ⣲ࡢ ᐃ࠿ࡽࡣ0Q㸪)H㸪$J㸪࡟ࡘ࠸࡚ࡶᅵተ࡬ࡢ⵳✚ࢆៅ㔜࡟᳨ウ
ࡍࡿᚲせࡀ࠶ࡿ࡜ᛮࢃࢀࡓࡀ  ᖺ࡜  ᖺࡢᅵተ୰ࡢඖ⣲ྵ᭷⋡࡟ࡣ  ࡘࡢヨ㦂༊㛫࡛᭷ពᕪࡀㄆ
ࡵࡽࢀ࡞࠿ࡗࡓࡇ࡜࡟ࡘ࠸࡚ࡶ㸪ᖺḟኚືࡢᙳ㡪ࡀ࠶ࡿࡢ࠿ࡶ▱ࢀ࡞࠸ࠋ ᱂ᇵస≀୰ࡢඖ⣲᱂ᇵస≀࡛࠶ࡿ࢚ࣥࣂࢡࡢ✑࡜ࢽࣥࢪࣥࡢྍ㣗㒊࠾ࡼࡧ⓶ࡢศᯒ⤖ᯝࢆ⾲  ࡟♧ࡋࡓࠋ࢚ࣥࣂࢡࡢ✑࠿ࡽࡣ 1D㸪0J㸪&O㸪.㸪&D㸪6F㸪&U㸪0Q㸪)H㸪&R㸪=Q㸪%U㸪5E ࡢ  ඖ⣲ࡀ᳨ฟࡉࢀࡓࠋ
࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࡛ࡣ &O ࡜ =Q ࡟ࡘ࠸࡚㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊࡛ࡣ =Q ࡜ %U ࡟ࡘ࠸࡚໬
Ꮫ⫧ᩱ༊ࡼࡾࡶඖ⣲ྵ᭷⋡ࡀ᭷ព࡟㧗ࡃ࡞ࡗࡓࠋࢥ
࣏ࣥࢫࢺࡢᢞධ࡟ࡼࡗ࡚ྵ᭷⋡ࡀ໬Ꮫ⫧ᩱࢆᢞධࡋ
ࡓሙྜࡼࡾࡶ㧗ࡃ࡞ࡗࡓࠋ&O ࡟ࡘ࠸࡚ࡣ⎔ቃ୰࡟ᗈࡃศᕸࡍࡿࡇ࡜㸪%U ࡟ࡘ࠸࡚ࡣ⡿㸪㯏㸪㞧✐ࡢṧ␃ᇶ‽್㸦ࠥPJNJ㸧㸧ࢆୗᅇࡗ࡚࠸ࡿࡇ࡜࠿ࡽ㸪ேయ࡟ᑐࡍࡿᏳ඲ᛶ࡟ࡣၥ㢟ࡀ࡞࠸࡜⪃࠼ࡽࢀࡿࠋ
=Q ࡟ࡘ࠸࡚ࡣ㸪㣗ရࡢᚤ㔞ඖ⣲ྵ㔞⾲  ࡟ࡼࢀࡤ㸪㻙㻌 㻟㻣㻝㻌㻙

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JAEA-Review 2011-050

ᶆ‽ⓗ࡞࢚ࣥࣂࢡࡢ⋞✐ࡢ =Q ྵ᭷㔞ࡣ᪂㩭㔜 J࠶ࡓࡾ PJ ࡛࠶ࡾ㸪஝≀ᙜࡓࡾ࡟᥮⟬ࡍࢀࡤ PJ
NJ ࡟┦ᙜࡍࡿࠋᮏᐇ㦂࡟࠾ࡅࡿ࢚ࣥࣂࢡࡢ✑ࡢ =Qྵ᭷⋡ࡣ㸪໬Ꮫ⫧ᩱ༊㸦=QPJNJ㸧࡟࠾࠸࡚ᶆ‽ࣞ࣋ࣝࢆⱝᖸୖᅇࡗ࡚࠸ࡓࠋࡲࡓ㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࡜࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊ࡢ =Qྵ᭷⋡ࡣᶆ‽ࣞ࣋ࣝࡢ࡯ࡰ  ಸ࡟┦ᙜࡋࡓࠋᅜẸᰤ㣴ㄪᰝ࡟ࡼࡿᡂே⏨ዪࡢࡑࡢ௚ࡢ✐㢮ࡢ  ᪥ᦤྲྀ㔞㸦J㸧 ࡜㣗ရࡢᚤ㔞ඖ⣲ྵ㔞⾲  ࡟࠶ࡿỈศ㔞ࢆᇶ࡟࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊ࡢ࢚ࣥࣂࢡࡢ✑ࢆJ ႚ㣗ࡋࡓሙྜࡢ =Q 㔞ࢆ⟬ฟࡋࡓሙྜ㸪ࡑࡢ್ࡣ ȣJ ࡜࡞ࡾ㸪᪥ᮏேࡢ =Q ࡢ  ᪥ᦤྲྀ㔞㸦PJ㸧࡟༨ࡵࡿ๭ྜࡣ⣙ 㸣࡜ᑡ࡞࠿ࡗࡓ㸦⾲㸧 ࠋࡲࡓ㸪ࣛࢵࢺ࡟ᑐࡍࡿሷ໬ள㖄ࡢ /' ࡣ PJ
NJ ࡛࠶ࡿࡇ࡜࠿ࡽࡶ㸪 ᖺ㛫ࡢ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺࡸ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝࡟ࡼࡗ࡚࢚ࣥ
ࣂࢡࡢ✑ࡢ =Q ྵ᭷⋡ࡀ໬Ꮫ⫧ᩱ᪋⏝᫬ࡼࡾࡶ㧗ࡃ࡞ࡗࡓ࡜ࡋ࡚ࡶ㣗ရ࡜ࡋ࡚Ᏻ඲ᛶ࡟ࡣၥ㢟ࡢ࡞࠸Ỉ‽࡟࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋ
୍᪉㸪ࢽࣥࢪࣥࡢሙྜ㸪⓶࠿ࡽࡣ 1D㸪0J㸪&O㸪.㸪
&D㸪6F㸪&U㸪0Q㸪)H㸪&R㸪=Q㸪%U㸪5E㸪6U㸪&V㸪%D㸪
/D㸪6P㸪(X㸪<E㸪/X ࡀ᳨ฟࡉࢀࡓࠋ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊㸼໬Ꮫ⫧ᩱ༊ࡢ㛵ಀࡀㄆࡵࡽࢀࡓඖ⣲ࡣ
0J㸪6F㸪0Q㸪=Q㸪%U㸪%D㸪/D ࡢ  ඖ⣲࡛࠶ࡾ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊㸼໬Ꮫ⫧ᩱ༊ࡢ㛵ಀࡣ 0J㸪0Q㸪
%U ࡢ  ඖ⣲࡟ㄆࡵࡽࢀࡓࠋ
ྍ㣗㒊࡟ࡘ࠸࡚ࡣ 1D㸪0J㸪
&O㸪.㸪&D㸪0Q㸪)H㸪&R㸪=Q㸪%U㸪5E㸪6U㸪&V㸪%Dࡢ  ඖ⣲ࡀ᳨ฟࡉࢀࡓࠋ=Q ࡜ 0Q ࡟ࡘ࠸࡚ࡣ࢜࢞ࢡ
ࢬởἾࢥ࣏ࣥࢫࢺ༊Ҹ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊㸼໬Ꮫ⫧ᩱ༊ࡢ㛵ಀࡀ㸪)H ࡜ &R ࡟ࡣ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊㸼໬Ꮫ⫧ᩱ༊ࡢ㛵ಀࡀ㸪&O ࡜ %U ࡟ࡣ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊㸼໬Ꮫ⫧ᩱ༊ࡢ㛵ಀࡀㄆࡵࡽࢀࡓࠋከࡃࡢඖ⣲ࡢྵ᭷⋡ࡀྍ㣗㒊ࡼࡾࡶ⓶࡟࠾࠸࡚㧗࠸್ࢆ♧ࡋࡓࡇ࡜࠿ࡽ㸪ࢥ࣏ࣥࢫࢺࢆᢞධࡋࡓᅵ
ተ࡛᱂ᇵࡋࡓࢽࣥࢪࣥ࠿ࡽࡢ୙せ࡞ඖ⣲ࡢேయ࡬ࡢ
ὶධࢆ㍍ῶࡍࡿࡓࡵ࡟ࡣ⓶ࡸ࡬ࡓ➼ࡢ㠀ྍ㣗㒊ࡢ㝖ཤࡀ᭷ຠ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋ㣗ရࡢᚤ㔞ඖ⣲ྵ㔞⾲  ࡟ࡼࢀࡤ㸪ࢽࣥࢪࣥࡢ =Q ࡜ 0Q ࡢྵ᭷㔞ࡣ᪂㩭㔜 J ࠶ࡓࡾ ȣJ ࡛࠶ࡾ㸪஝≀ᙜࡓࡾ࡛ࡣ PJ
NJ ࡟┦ᙜࡍࡿࠋࡇࡢ್ࢆᶆ‽ⓗ࡞ࢽࣥࢪࣥࡢ್࡜
ࡋࡓሙྜ㸪ᮏᐇ㦂࡟࠾ࡅࡿࢽࣥࢪࣥࡢྍ㣗㒊ࡢ =Q
࡜ 0Q ࡢྵ᭷⋡ࡣ㸪໬Ꮫ⫧ᩱ༊㸦=QPJNJ㸪
0QPJNJ㸧࡟࠾࠸࡚ =Q ࡣᶆ‽ࣞ࣋ࣝࢆ᪤࡟
ୖᅇࡗ࡚࠸ࡿࡀ㸪0Q ࡣᶆ‽ࣞ࣋ࣝࢆୗᅇࡗ࡚࠸ࡓࠋ
࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࡜࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫ
ࢺ༊ࡢࢽࣥࢪࣥࡢྍ㣗㒊ࡢ =Q ࡜ 0Q ࡢྵ᭷⋡ࡣᶆ‽ࣞ࣋ࣝࡢ  ಸ௨ෆ࡛࠶ࡗࡓࠋ)H ࡢሙྜ㸪㣗ရᶆ‽ᡂศ⾲  ࠿ࡽồࡵࡓ஝≀࠶ࡓࡾࡢྵ᭷⋡ࡣ⣙ PJNJ
࡛࠶ࡗࡓࡢ࡛㸪ᮏᐇ㦂࡟࠾ࡅࡿࢽࣥࢪࣥࡢྍ㣗㒊ࡢྵ᭷⋡ࡣ㸪࠸ࡎࢀࡢ༊ࡶᶆ‽ࣞ࣋ࣝࢆୗᅇࡗ࡚࠸ࡓࠋ
&R ࡟ࡘ࠸࡚ࡣᚤ㔞ඖ⣲ྵ㔞⾲  ࠿ࡽồࡵࡓ஝≀ᙜࡓࡾࡢྵ᭷⋡ࡀ PJNJ ࡛࠶ࡿࡓࡵ㸪ᮏᐇ㦂࡟࠾ࡅࡿ&R ྵ᭷⋡㸦໬Ꮫ⫧ᩱ༊ PJNJ㸧ࡣᶆ‽ⓗ࡞ࢽࣥࢪࣥࡼࡾࡶ㧗࠸࡜⪃࠼ࡽࢀࡓࠋᅜẸᰤ㣴ㄪᰝ࡟ࡼࡿᡂே⏨ዪࡢࢽࣥࢪࣥࡢ  ᪥ᦤྲྀ㔞㸦J㸧 ࡜㣗ရࡢᚤ㔞ඖ⣲ྵ㔞⾲  ࡟࠶ࡿỈศ㔞ࢆᇶ࡟࢜࢞ࢡࢬ
ởἾࢥ࣏ࣥࢫࢺ༊ࡢࢽࣥࢪࣥࡢྍ㣗㒊ࢆ J ႚ㣗ࡋࡓሙྜࡢ =Q㸪0Q㸪)H㸪&R 㔞ࢆ⟬ฟࡋࡓሙྜ㸪ࡑࡢ್ࡣࡑࢀࡒࢀ ȣJ㸪ȣJ㸪ȣJ㸪ȣJ࡜࡞ࡗࡓ㸦⾲ 㸧ࠋࡇࢀࡽࡢ್ࡢ᪥ᮏேࡢ =Q ࡜ 0Q ࡢ ᪥ᦤྲྀ㔞  㸪ᪧཌ⏕┬ࡢᐃࡵࡓ )H ࡢ  ᪥ᡤせ㔞  㸪㤶ᕝ┴࡟࠾ࡅࡿேࡢ &R ࡢ  ᪥ᦤྲྀ㔞  ࡟༨ࡵࡿ๭ྜ
࡛ࡣ =Q ࡛⣙ 㸣㸪0Q ࡛⣙ 㸣㸪)H ࡛⣙ ࠥ㸣㸪&R ࡛⣙ 㸣࡜࡞ࡾ 0Q ࡸ &R ࡟ࡘ࠸࡚ࡣ =Q ࡸ )H ࡼ
ࡾࡶ  ᪥ᦤྲྀ㔞  ࡟༨ࡵࡿ๭ྜࡀࡸࡸ㧗࠸ഴྥࡀㄆ
ࡵࡽࢀࡓࠋࡋ࠿ࡋ㸪ࣛࢵࢺ࡟ᑐࡍࡿሷ໬ள㖄㸪ሷ໬࣐ࣥ࢞ࣥ㸪ሷ໬➨୍㕲㸪ሷ໬ࢥࣂࣝࢺࡢ /' ࡣ PJ
NJ㸪PJNJ㸪PJNJ㸪PJNJ ࡛࠶ࡿࡇ࡜࠿ࡽ㸪ᮏ◊✲࡟࠾࠸࡚ࡣ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫ
ࢺࡸ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࢆ  ᖺ⛬ᗘ᪋⏝ࡍࢀࡤࢽࣥࢪࣥࡢྍ㣗㒊ࡢ =Q㸪0Q㸪)H㸪&R ࡢྵ᭷⋡ࡀ໬Ꮫ⫧ᩱ༊ࡼࡾࡶ㧗ࡃ࡞ࡿࡇ࡜ࡀ࠶ࡗ࡚ࡶ㸪Ᏻ඲ᛶࡢⅬ࡛ࡣၥ㢟ࡢ࡞࠸Ỉ‽࡛࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋࡲࡓ㸪࣑ࣔ࢞ࣛࢥ࣏ࣥࢫࢺ༊ࡢࢽࣥࢪࣥྍ㣗㒊ࡢ &O ࡜ %U ࡢྵ᭷⋡࡟ࡘ࠸࡚ࡶ㸪࢚ࣥࣂࢡࡢ✑ࡢሙྜ࡜ྠᵝ࡞⌮⏤࡛㸪ேయ࡟ᑐࡍࡿᏳ඲ᛶ࡛ࡣၥ㢟ࡀ࡞࠸ࣞ࣋ࣝ࡜
⪃࠼ࡽࢀࡓࠋ
௨ୖࢆࡲ࡜ࡵࡿ࡜㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫ
ࢺࡸ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࢆ  ᖺ㛫᪋⏝ࡍࡿࡇ࡜࡟ࡼࡗ࡚㸪᱂ᇵస≀ࡢ 0Q ࡸ =Q ➼ࡢඖ⣲ࡢྵ᭷⋡ࡀ໬Ꮫ⫧ᩱࢆ᪋⏝ࡋࡓሙྜࡼࡾࡶ㧗ࡃ࡞ࡿࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡗࡓࠋࡋ࠿ࡋ㸪㣗ရ࡜࡞ࡿ࢚ࣥࣂࢡࡢ✑ࡸࢽࣥࢪࣥࡢྍ㣗㒊࡛ࡣ㸪ởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝࡟ࡼࡗ࡚ඖ⣲ࡢྵ᭷⋡ࡀቑຍࡋ࡚ࡶ㸪Ᏻ඲ᛶࡢⅬ࡛ࡣၥ㢟ࡀ࡞࠸Ỉ‽࡛࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋせ⣙〓Ⰽ᳃ᯘᅵࡢ⏿ᅡሙ࡟  ✀㢮ࡢୗỈởἾࢥ࣏ࣥࢫࢺ㸦࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ࡜࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ㸧ࢆ  ᖺ㛫᪋⏝ࡋ㸪ᅵተ࡜᱂ᇵస≀ ࢚ࣥࣂࢡ࡜ࢽࣥࢪࣥ ࡟ྵࡲࢀࡿᵝࠎ࡞ඖ⣲ࡢ㔞ࢆ໬Ꮫ⫧ᩱࡢࡳࢆ᪋⏝ࡋࡓሙྜ࡜ẚ㍑ࡋࡓࠋ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ࡟ࡣ 0Q㸪)H㸪=Q㸪$J㸪%D㸪/D㸪&H ࡀ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ࡟ࡣ 0Q㸪=Q㸪㻙㻌 㻟㻣㻞㻌㻙

4-7

JAEA-Review 2011-050$J㸪%D ࡀ໬Ꮫ⫧ᩱ࡜ẚ࡭࡚㸵ಸ௨ୖ㧗࠸ྵ᭷⋡࡛ྵࡲࢀ࡚࠸ࡓࠋ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊㸪໬Ꮫ⫧ᩱ༊ࡢᅵተࡢྛඖ⣲ࡢྵ᭷⋡ࢆẚ㍑ࡋࡓ⤖ᯝ㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺࡸࣔ
࣑࢞ࣛởἾࢥ࣏ࣥࢫࢺࢆ〓Ⰽ᳃ᯘᅵ࡟  ᖺ㛫ᢞධࡋࡓ㝈ࡾ࡟࠾࠸࡚ࡣ㸪=Q㸪$V㸪6E㸪%D㸪/D㸪&H ࡀᅵተ࡟⵳✚ࡋࡸࡍ࠸ྍ⬟ᛶࡀ࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋ
࢚ࣥࣂࢡࡢ✑࡟ࡘ࠸࡚ࡣ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫ
ࢺࡢ᪋⏝࡟ࡼࡗ࡚ 0J㸪&O㸪&D㸪=Q ࡢྵ᭷⋡ࡀ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝࡟ࡼࡗ࡚ 0J㸪&D㸪=Q㸪%U
ࡢྵ᭷⋡ࡀ໬Ꮫ⫧ᩱࡢࡳࢆ᪋⏝ࡋࡓሙྜࡼࡾࡶ᭷ព
࡟㧗ࡃ࡞ࡗࡓࠋࡲࡓ㸪ࢽࣥࢪࣥࡢྍ㣗㒊࡟ࡘ࠸࡚ࡣ
࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝࡟ࡼࡗ࡚ 0Q㸪)H㸪=Q㸪
&R㸪%U ࡢྵ᭷⋡ࡀ㸪࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺࡢ᪋⏝࡟ࡼࡗ࡚ &O㸪0Q㸪=Q㸪%U ࡢྵ᭷⋡ࡀ໬Ꮫ⫧ᩱࡢࡳࢆ᪋⏝ࡋࡓሙྜࡼࡾࡶ᭷ព࡟㧗ࡃ࡞ࡗࡓࠋ
ୗỈởἾࢥ࣏ࣥࢫࢺ᪋⏝ࡋࡓሙྜࡢ࢚ࣥࣂࢡࡢ
✑ࡸࢽࣥࢪࣥྍ㣗㒊ࡢ 0Q㸪)H㸪=Q㸪&R ࡢྵ᭷⋡࡟ࡘ࠸࡚Ᏻ඲ᛶࢆ᳨ウࡋࡓ⤖ᯝ㸪 ᪥ᦤྲྀ㔞࡟ᑐࡍࡿ㔞ࡸࣛࢵࢺ࡟ࡼࡿ /' ࡢⅬ࠿ࡽ㣗ရ࡜ࡋ࡚ࡢᏳ඲ᛶ࡟
ၥ㢟ࡣ࡞࠸Ỉ‽࡛࠶ࡿ࡜⪃࠼ࡽࢀࡓࠋ
㸦4㸧௒ᚋࡢ᪉㔪 ᖺ࡜  ᖺࡢᅵተࡢඖ⣲ྵ᭷⋡ࢆẚ㍑ࡍࡿ
࡜㸪=Q ࡢࡼ࠺࡟ᢞධ㔞࡜ࡋ࡚ࡣ  ᖺࡢ᪉ࡀከ࠸
࡟ࡶ࠿࠿ࢃࡽࡎ  ᖺࡢ᪉ࡀ㧗࠸ഴྥࢆ♧ࡋ࡚࠸ࡿሙྜࡶ࠶ࡿࠋࡇࡢࡓࡵ㸪ᅵተ࡟࠾ࡅࡿඖ⣲ࡢ⵳✚ࢆṇ☜࡟ᢕᥱࡍࡿࡓࡵ࡟ࡣከᖺᗘ࡟ࢃࡓࡿᖺḟኚື࡟ࡘ࠸࡚ࢹ࣮ࢱࢆ㞟ࡵࡿᚲせࡀ࠶ࡿࠋ↓ᶵඖ⣲ࡢᦤྲྀ㔞࡟ࡘ࠸࡚㸦➨㸰ሗ㸧㸪㤶ᕝ┴⎔ቃಖ೺◊✲ࢭࣥࢱ࣮ᡤሗ㸪㸪ࠥ㸦㸧㸧⛉Ꮫᢏ⾡ᗇ㈨※ㄪᰝ఍⦅㸸ᅄゞ᪥ᮏ㣗ရᶆ‽ᡂศ
⾲㸪Sࠥ㸪኱ⶶ┬༳ๅᒁ㸪ᮾி㸦㸧㸧ẟ฼Ꮥ࣭᫂すᒸ༓㭯࣭▼ᕝⱥᶞ࣭㯮⏣ᘯஅ㸸㤶ᕝ┴࡟࠾ࡅࡿ᪥ᖖ㣗ရ୰ࡢ㔠ᒓࡢ୍᪥ᦤྲྀ㔞࡟ࡘ࠸࡚㸪㤶ᕝ┴⾨⏕◊✲ᡤሗ㸪㸪ࠥ㸦㸧
㸦6㸧ᡂᯝࡢබ⾲㸦ㄽᩥ㸧6X]XNL+6X]XNL<.XPDJDL+1RJDZD1
.DZDWH06DZDKDWD+6DNDPRWR.DQG
,QXEXVKL . ,QIOXHQFH RI VHZDJH VOXGJHFRPSRVWDSSOLFDWLRQVRQXSWDNHRIHOHPHQWE\FXOWLYDWHGFURSVLQDEURZQIRUHVWVRLO̾PHDVXUHPHQW E\ WKH QHXWURQ DFWLYDWLRQDQDO\VLV ̾  5DGLRLVRWRSHV  
 
2JL\DPD66DNDPRWR.6X]XNL+8VKLR6
$Q]DL7DQG,QXEXVKL.0HDVXUHPHQWRI
FRQFHQWUDWLRQV RI WUDFH PHWDOV LQ DUDEOH
VRLOVZLWKDQLPDOPDQXUHDSSOLFDWLRQXVLQJLQVWUXPHQWDO QHXWURQ DFWLYDWLRQ DQDO\VLV
DQGWKHFRQFHQWUDWHGDFLGGLJHVWLRQPHWKRG
6RLO 6FLHQFH DQG 3ODQW 1XWULWLRQ   㸦5㸧ᘬ⏝ᩥ⊩ 㕥ᮌᘯ⾜࣭ᮧᯇ㞞Ꮚ࣭㕥ᮌᝆ୍࣭Ⲷᒣៅ୍࣭⇃㇂ᏹ࣭㔝ᕝ᠇ኵ㸸࢔࣮ࣂࢫ࣮࢟ࣗࣛ⳦᰿ࢆᙧᡂ
ࡋࡓ᳜≀ࡢᚤ㔞ඖ⣲ศᯒ࡜᳜≀ಖㆤᢏ⾡࡜ࡋ࡚ࡢ࢔࣮ࣂࢫ࣮࢟ࣗࣛ⳦᰿⳦ࡢ฼⏝ྍ⬟ᛶࡢ᳨ウཎ◊᪋タ฼⏝ඹྠ◊✲ᡂᯝሗ࿌᭩
  㸧ᰗ஭ஂỤ㸸6WHS ࢚ࢡࢭࣝ⤫ィ㸪Sࠥ㸪࣮࢚࣒࢚࢜ࢫฟ∧㸪ᡤἑ㸦㸧㸧㎰⸆ṧ␃ศᯒἲ◊✲⌜㸸᭱᪂㎰⸆ࡢṧ␃ศᯒἲ㸪Sࠥ㸪୰ኸἲつฟ∧㸪ᮾி㸦㸧㸧㕥ᮌὈኵ⦅㸸㣗ရࡢᚤ㔞ඖ⣲ྵ㔞⾲㸪➨୍ฟ∧㸪ᮾி㸦㸧㸧ྜྷụಙ⏨㸸ṧ␃㎰⸆ࡢᭀ㟢㔞ヨ⟬ࡢࡓࡵࡢ㣗ရᦤྲྀ㔞ᇶ‽ࢹ࣮ࢱࡢ᳨ウѸ ࠥ ᖺᅜẸᰤ㣴ㄪᰝ㸪㣗ရ⾨⏕◊✲㸪㸪ࠥ㸦㸧㸧すᒸ༓㭯࣭ྜྷ⏣᫂⨾࣭⸨⏣ஂ㞝࣭ẟ฼Ꮥ࣭᫂ሯᮏ
Ṋ࣭㯮⏣ᘯஅ㸸㤶ᕝ┴࡟࠾ࡅࡿ᪥ᖖ㣗ရ୰ࡢ㻙㻌 㻟㻣㻟㻌㻙

4-7

JAEA-Review 2011-050

⾲ࠉྛヨ㦂༊࡬ࡢୗỈởἾࢥ࣏ࣥࢫࢺ࠾ࡼࡧ໬Ꮫ⫧ᩱࡢ᪋⏝㔞࡜᱂ᇵస≀᪋⏝㔞㸦WKD᱂ᇵᅇᩘ᪋⏝࠾ࡼࡧ᧛✀ᖺ᭶ ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࠾ࡼࡧ࣑ࣔ
࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

໬Ꮫ⫧ᩱ༊

᱂ᇵస≀

໬Ꮫ⫧ᩱ










࢚ࣥࣂࢡ
኱㇋
࢚ࣥࣂࢡ
ࢽࣥࢪࣥ
࢚ࣥࣂࢡ
ࢽࣥࢪࣥ
࢔ࣝࣇ࢓ࣝࣇ࢓
ࢧࢶ࣐࢖ࣔ↓స௜࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ
ࡲࡓࡣ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ



















㹼㸧











໬Ꮫ⫧ᩱ










⾲ࠉ↷ᑕ᮲௳࠾ࡼࡧ ᐃ᰾✀↷ᑕཎᏊ⅔㸦タഛ㸧᭱኱⇕୰ᛶᏊ᮰
P ࣭V 

↷ᑕ᫬㛫

෭༷᫬㛫

ᐃヨᩱ

⛊
⛊

㹼ศ
㹼ศ

ᅵተ㸪ྛởἾࢥ࣏ࣥࢫࢺ㸬໬Ꮫ⫧ᩱ࢚ࣥࣂࢡ㸪ࢽࣥࢪࣥ

-55㸦7ࣃ࢖ࣉ$㸧
ࡲࡓࡣ-550 31  

ศ
ศ

㐌㛫
㐌㛫

඲ヨᩱ

1D  1D .  . 6F  6F &U &U 
)H  )H &R  &R =Q  =Q $V  $V 
%U  %U 5E  5E 6U 6U =U =U $J P $J 6E  6E &V  &V %D  %D 
/D  /D &H  &H 6P  6P (X  (X <E  <E /X  /X 7D  7D 7K  3D 
8  1S

-55㸦7ࣃ࢖ࣉ$㸧
ࡲࡓࡣ-550 31  

ศ
ศ

㹼ࣨ᭶
㹼ࣨ᭶

඲ヨᩱ

$J P $J-55㸦Ẽ㏦⟶㸧

ᐃඖ⣲㸦

ᐃ᰾✀㸧

&O  &O &D &D 0J  0J 0Q

0Q

⾲ࠉୗỈởἾࢥ࣏ࣥࢫࢺ࠾ࡼࡧ໬Ꮫ⫧ᩱ୰ࡢඖ⣲ྵ᭷㔞࡜ୗỈởἾࢥ࣏ࣥࢫࢺ࡟⏤᮶ࡍࡿඖ⣲ࡢ⌮ㄽቑຍ㔞ୗỈởἾࢥ࣏ࣥࢫࢺ࡟⏤᮶ࡍࡿୗỈởἾࢥ࣏ࣥࢫࢺ࠾ࡼࡧ໬Ꮫ⫧ᩱඖ⣲ඖ⣲ࡢ⌮ㄽቑຍ㔞ࠉ PJNJ  ':
PJNJ  ':࢜࢞ࢡࢬởἾ
࣑ࣔ࢞ࣛởἾ
໬Ꮫ⫧ᩱ࢜࢞ࢡࢬởἾ
࣑ࣔ࢞ࣛởἾ
ࢥ࣏ࣥࢫࢺ

ࢥ࣏ࣥࢫࢺ

ࢥ࣏ࣥࢫࢺ༊

1D


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0J
   


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.
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
6F
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
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&U
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

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0Q
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

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   

&R


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=Q
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%U
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5E
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6U
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
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6E
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7K
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8
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 ᪋⏝ࡋࡓୗỈởἾࢥ࣏ࣥࢫࢺ୰ࡢඖ⣲ࡀ඲࡚సᅵᒙ㸦㹼FP㸧࡟␃ࡲࡗࡓሙྜ࡟ᅵተᐦᗘࢆ

ࠉNJP࡜௬ᐃࡋ࡚⟬ฟࡋࡓ㻙㻌 㻟㻣㻠㻌㻙

ࢥ࣏ࣥࢫࢺ༊

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

4-7

JAEA-Review 2011-050

⾲ࠉᖺ࡜ᖺ࡟᥇ྲྀࡋࡓྛヨ㦂༊࡟࠾ࡅࡿᅵተ୰ࡢྛ✀ඖ⣲ྵ᭷⋡
ඖ⣲

ヨ㦂༊

1D

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

0J

&O

.

&D

&U

0Q

)H

&R

=Q

$V

%U

5E

6U

D

ඖ⣲

ヨ㦂༊



=U

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

  s  D  s   D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D

 s 

D

໬Ꮫ⫧ᩱ༊

  s  D  s   D໬Ꮫ⫧ᩱ༊ s D s D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

  s  D  s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

  s  D  s  ໬Ꮫ⫧ᩱ༊  s  D  s  ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s ໬Ꮫ⫧ᩱ༊ s D s 





1'

1'

D

࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

1'

1'

D

໬Ꮫ⫧ᩱ༊

1'

6E

1'

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  E

D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  DE

D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D  s   D  s   D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D  s  D  s   D໬Ꮫ⫧ᩱ༊ s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

  s  D  s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s 

E࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

  s  D  s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s DE s 





D

&V

 s 

࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s 

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊



D



$J

໬Ꮫ⫧ᩱ༊

D

 s 

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s ໬Ꮫ⫧ᩱ༊ s D s ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s 

D

໬Ꮫ⫧ᩱ༊

 s D s 

D

໬Ꮫ⫧ᩱ༊

6F


  s   D  s  

㸧

D

໬Ꮫ⫧ᩱ༊

 s D s 

D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s ED࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s 

D

D

໬Ꮫ⫧ᩱ༊

 s D s D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s E࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s 

D

໬Ꮫ⫧ᩱ༊

 s D s D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D໬Ꮫ⫧ᩱ༊ s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

  s   D  s   D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

  s   D  s   D



໬Ꮫ⫧ᩱ༊

 s 

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊





%D



/D

&H

6P

D

 s 

D  s  D  s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

  s  D  s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D໬Ꮫ⫧ᩱ༊  s  D  s  

D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D໬Ꮫ⫧ᩱ༊ s D s 

D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s E

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s E

࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D໬Ꮫ⫧ᩱ༊ s D s D

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s 

D

(X

<E

/X

7D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s E

࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D໬Ꮫ⫧ᩱ༊ s D s 

D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D

 s D

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D

 s D

࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D

 s  D໬Ꮫ⫧ᩱ༊ s D

 s 

D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s E s D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s D࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s  D໬Ꮫ⫧ᩱ༊ s DE s 

D

໬Ꮫ⫧ᩱ༊

 s D s  D࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

 s D s D

࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

 s D s D໬Ꮫ⫧ᩱ༊ s D s D

7K

8

⾲୰ࡢ್ࡣᖹᆒ್࡜ᶆ‽೫ᕪ㸦Q  ࡲࡓ⾲୰ࡢⱥᩥᏐࡣ%RQIHUURQL'XQQἲ࡟ࡼࡿ⤫ィฎ⌮⤖ᯝࢆ♧ࡍ㸦ྠ୍ⱥᩥᏐࡣS㸺࡛ྠ୍ᖺᗘࡢヨ㦂༊㛫࡛᭷ពᕪࡀ࡞࠸ࡇ࡜ࢆ♧ࡍ 㸪1'㸸᳨ฟ㝈⏺௨ୗ

4-7

㻙㻌 㻟㻣㻡㻌㻙

JAEA-Review 2011-050

⾲ࠉྛヨ㦂༊࡟࠾࠸࡚᱂ᇵࡋࡓ࢚ࣥࣂࢡࡢ✑࠾ࡼࡧࢽࣥࢪࣥࡢྍ㣗㒊࡜⓶ࡢྛ✀ඖ⣲ྵ᭷⋡ D࢚ࣥࣂࢡࡢ✑
ඖ⣲࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

PJNJ':࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

໬Ꮫ⫧ᩱ༊ࠉࠉࢽࣥࢪࣥࡢྍ㣗㒊࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊

PJNJ':࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

ࠉࠉࢽࣥࢪࣥࡢ⓶໬Ꮫ⫧ᩱ༊

1D s D s D s D s D s D s   s   D  s   D  s   D  s   D  s  
0J  s   D  s   D  s   D  s   D  s   E  s  &O  s   E










 s  D s 
D
 s 
D s 
D  s  .
 s  D  s   D  s   D  s   D  s   D  s  &D  s   D
6F s 
D s 
D s 
E
1'
1'
1'
&U
 s D s D s 
D
1'
1'
1'
0Q
 s D s D s D s E s E s )H s D s D s E s E s D s &R s E s D s DE s 
E s 
DE s 
=Q
 s F s E s D s E s E s 
1'
1'
1'
1'
1'
1'
$V
%U
 s D s E s D s D s E s 5E
 s E s D s E s E s D s 
1'
1'
1'
6U
 s D s D s 
1'
1'
1'
1'
1'
1'
=U
1'
1'
1'
1'
1'
1'
$J
1'
1'
1'
1'
6E
1'
1'
1'
1'
1'
D
 s 
&V s 
D s 
%D s E s D s 
1'
1'
1'
1'
1'
1'
/D
1'
1'
1'
1'
1'
1'
&H
1'
1'
1'
1'
1'
1'
6P
1'
1'
1'
1'
1'
1'
(X
1'
1'
1'
1'
1'
1'
<E
1'
1'
1'
1'
1'
1'
/X
1'
1'
1'
1'
1'
1'
7D
1'
1'
1'
1'
1'
1'
1'
1'
1'
7K
1'
1'
1'
1'
1'
1'
8
D ⾲୰ࡢ್ࡣᖹᆒ್࡜ᶆ‽೫ᕪ㸦Q  ࡲࡓ⾲୰ࡢⱥᩥᏐࡣ%RQIHUURQL'XQQἲ࡟ࡼࡿ⤫ィฎ⌮⤖ᯝࢆ♧ࡍ㸦ྠ୍ⱥᩥᏐࡣS㸺࡛ヨ㦂༊㛫࡛᭷ពᕪࡀ࡞࠸ࡇ࡜ࢆ♧ࡍ 㸪1'㸸᳨ฟ㝈⏺௨ୗ

PJNJ':࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊

࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊
D
D
D
D
D

D
D
D
D
D
E
D

D
DE

 s   s    s    s    s   s 
 s 
 s  s  s 
 s 
1' s  s  s 1'1'1' s 
 s  s 
1' s 
 s 
 s 
 s 
1'
1'
1'

DE
E
D
D
D
E
D
F
D
D
E
E
DE
E

D
E
E
D
D
D
D

 s   s    s    s    s   s 
 s 
 s  s  s 
 s 
1' s  s  s 1'1'1' s 
 s  s 
1' s 
 s 
 s 
 s 
1'
1'
1'

໬Ꮫ⫧ᩱ༊
D
E
D
DE
D
DE
D
E
D
D
D
F
D
D

D
D
D
D
D
D
D

⾲ࠉ=Q0Q)H&Rࡢ᪥ᦤྲྀ㔞࡜࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊ࡢ࢚ࣥࣂࢡࡢ✑ࠉࠉ࠾ࡼࡧࢽࣥࢪࣥࡢྍ㣗㒊࠿ࡽࡢ᥎ᐃᦤྲྀ㔞ᮏᐇ㦂ࡢ࢚ࣥࣂࢡࢆ
ᮏᐇ㦂ࡢࢽࣥࢪࣥࢆ
D㸧a)
1日の摂取量Jႚ㣗ࡋࡓሙྜࡢ Jႚ㣗ࡋࡓሙྜࡢ
ඖ⣲ࠉ᪥ᦤྲྀ㔞
E㸧 b)
F㸧 d)
1日の摂取量
1日の摂取量ྛඖ⣲ࡢ᪥ᦤྲྀ㔞ྛඖ⣲ࡢ᪥ᦤྲྀ㔞=QPJȣJ
ȣJ
ȣJ
0Q
PJ
ࠉ̿G㸧
)H⏨ࠉPJ̿ȣJ
ዪࠉPJ&RȣJ̿ȣJ
平均値
D =Q࠾ࡼࡧ0Q㹼ᖺࡲ࡛ࡢ᪥ᮏே࡟ࡼࡿඖ⣲ࡢ୍᪥ᦤྲྀ㔞ࡢᖹᆒ್㸧
要量㸪&R㹼ᖺࡲ࡛ࡢ㤶ᕝ┴࡟࠾ࡅࠉ)Hᪧཌ⏕┬ࡀᐃࡵࡓ᪥ᡤせ㔞
平均値ࡿேࡢ୍᪥ᦤྲྀ㔞ࡢᖹᆒ
1日の摂取量（0.294g）食品のE ᅜẸᰤ㣴ㄪᰝ࡟ࡼࡿᡂே⏨ዪࡢࡑࡢ௚ࡢ✐㢮ࡢ᪥ᦤྲྀ㔞J㸪㣗ရࡢ区ࠉᚤ㔞ඖ⣲ྵ㔞⾲࡟࠶ࡿỈศ㔞 J࠶ࡓࡾJ 㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊
ࠉࡢ࢚ࣥࣂࢡࡢ✑ࡢྛඖ⣲ྵ᭷⋡ࢆᇶ࡟⟬ฟࡋࡓ
1日の摂取量（85.4g）食品の微量F ᅜẸᰤ㣴ㄪᰝ࡟ࡼࡿᡂே⏨ዪࡢࢽࣥࢪࣥࡢ᪥ᦤྲྀ㔞
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ࠉඖ⣲ྵ㔞⾲࡟࠶ࡿỈศ㔞 J࠶ࡓࡾJ 㸪࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊ࡢ
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肥G ࢜࢞ࢡࢬởἾࢥ࣏ࣥࢫࢺ༊࠶ࡿ࠸ࡣ࣑ࣔ࢞ࣛởἾࢥ࣏ࣥࢫࢺ༊ࡢ್ࡀ໬Ꮫ⫧࡜ࡣ⤫ィⓗ࡟᭷ពᕪࢆ♧ࡉ࡞࠿ࡗࡓࡢ࡛⟬ฟࡋ࡞࠿ࡗࡓ

4-7

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JAEA-Review 2011-050
















5.  ߘߩઁ 

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JAEA-Review 2011-050

5-1⎇ⓥ࠹࡯ࡑ㧦ਛᕈሶ᝝ᝒ≮ᴺㆡᔕ≸⣲ߩᴦ≮ࡊࡠ࠻ࠦ㧙࡞ߩ⏕┙⴫   㗴㧦㗡㗪ㇱ≸ߦኻߔࠆ⎲⚛ਛᕈሶ᝝ᝒ≮ᴺ
Boron neutron capture therapy for head and neck malignancies.
ᐔႦ⚐৻‫☿ޔ‬㘵ේノੱ 㧝 ‫ޔ‬ቝ㊁㓷ሶ 㧝 ‫ޔ‬ᾢ↰ඳ᣿ 2‫ޔ‬ዊ㊁౏ੑ 3‫ޔ‬ේ↰଻ 㧝

Ꮉፒක⑼ᄢቇ᡼኿✢කቇ(ᴦ≮)
㧝Ꮉፒක⑼ᄢቇ⡊㥦ຜ༄⑼㧞ᣣᧄේሶജ㐿⊒ᯏ᭴
3 ੩ㇺᄢቇේሶἹታ㛎ᚲ
Departments of Radiation Oncology, and 1Otolaryngology Head and Neck Surgery,
Kawasaki Medical School, Kurashiki, Japan
2 Japan Atomic Energy Agency
3 Radiation Oncology Research Laboratory, Research Reactor Institute, Kyoto University,
Osaka, Japan㧔㧝㧕 ߪߓ߼ߦ㗡 㗪 ㇱ ≸ ᴦ ≮ ߪ ‫ޔ‬ᄖ ⑼ ⊛ ᴦ ≮ ‫ޔ‬᡼ ኿ ✢ᴦ ≮ ‫ޔ‬᛫ ≸ ೷ ᴦ ≮ ߩ 3 ⠪ ࠍ ⥋ ㆡ ߦ ⚵ ߺ วࠊߖࠆᣇᴺ߇ਥᵹߢ޽ࠆ‫ޕ‬ฦᴦ≮ᴺߩᛛ
ⴚߪᡷ⦟ߐࠇᴦ≹₸ߪะ਄ߒߡ߈ߡ޿ࠆ
߇‫߇⷗⊒ޔ‬ㆃࠇߚㅴⴕ≸߿ᴦ≮ᓟߩౣ⊒≸ߢߪ‫߇଀∝ߩߤࠎߣ߶ޔ‬ᓥ᧪ߩᴦ≮ᴺߢߩቢోᴦ≹ࠍᦼᓙߔࠆߎߣߪ㔍ߒ޿‫ޕ‬㗡㗪ㇱ߇ᯏ⢻਄࡮⟤ኈ਄ߘߩ᷷ሽ߇ᄢᄌ
㊀ⷐߥ㗔ၞߢ޽ࠅ‫ޔ‬ᓥ᧪ߩᴦ≮ᴺߢߪ‫ޔ‬೙ ᓮ ࿎ 㔍 ߣ ᕁ ࠊ ࠇࠆ ㅴ ⴕ ∛ Ꮍ ࡮ ౣ ⊒ ∛ ᎽࠍᱜᏱ⤳ེࠍ៊ߥ߁ߎߣߥߊᴦ≮ߢ߈ࠇ߫‫ޔ‬ᖚ⠪ߩᄢ߈ߥ⽶⩄ߪ൩⺰ߩߎߣᴦ≮ᓟ ߩ 㜞 ޿ QOL ߇ ᦼ ᓙ ߢ ߈ ࠆ ‫߁ ࠃ ߩ ߘ ޕ‬ߥᴦ≮ᴺ㐿⊒ߪࠃࠅ㊀ⷐ߆ߟᕆോߣߥࠆ‫ޕ‬ࠕࡒࡁ㉄ઍ⻢߇੣ㅴߒߚ≸⚦⢩ߦ․⇣⊛ ߦ 㓸 Ⓧ ߔ ࠆ p-boronophenylalanine(BPA)ࠍ ↪ ޿ ߚ ਛ ᕈ ሶ ᝝ ᝒ ≮ ᴺ 㧔 BNCT㧕ߪ ‫ޔ‬ਥ ߦ ≸ ⚵ ❱ ߦ 㓸 Ⓧ ߒ ߚ ⎲ ⚛㧔 10 B㧕ߣᾲ ਛ ᕈ ሶ ߣ ߩ ᩭ ෻ ᔕ ߢ ↢ ߓ ࠆ 㜞 LET ᡼኿ ✢ (ǩ ☸ ሶ )ߦ ࠃ ࠅ ≸ ⚦ ⢩ ߛ ߌ ߦ ࠛ ࡀ ࡞ࠡ㧙ࠍ㓸ਛߐߖࠆ੐߇น⢻ߢ޽ࠅ≸ᴦ≮ߦ ℂ ᗐ ⊛ ߢ ޽ ࠆ 1) ‫ ߚ ߹ޕ‬BPA ߩ ⣲ ≌ 㓸 Ⓧ
ߪ 18 F-BPA PET ߢ ߩ ቯ ㊂ ߇ น ⢻ ߢ ‫ߩ ߘޔ‬⚿ ᨐ ߆ ࠄ ᛫ ⣲ ≌ ല ᨐ ߇ ੍ ᷹ น ⢻ ߢ ޽ ࠆ 2) ‫ޕ‬ᚒ ‫ ߪ ޘ‬਄ ⸥ ℂ ⺰ ߦ ၮ ޿ ߡ ‫ ޔ‬2003 ᐕ 10᦬߆ࠄᎹፒක⑼ᄢቇ୶ℂᆔຬળᛚ⹺ߩ߽
ߣ‫ޔ‬ㅴⴕ㗡㗪ㇱ≸ᖚ⠪ߦਛᕈሶ᝝ᝒ≮ᴺࠍ ⴕ ߞ ߡ ߅ ࠅ ‫ ޔ‬2007 ᐕ ߦ BNCT ࠍ ⴕ ߞߚ∝଀ߩ⹦⚦ࠍႎ๔ߔࠆ‫ޕ‬㧔㧞㧕ኻ⽎ߣᣇᴺ
ኻ⽎ߪ 2007 ᐕ 1 ᦬߆ࠄ 2007 ᐕ 12 ᦬߹ߢߩ㑆ߦ‫(ޔ‬1)㗡㗪ㇱ≸ᮡḰᴦ≮ߦߡ೙ᓮ࿎
㔍‫ޔߪߚ߹ޔ‬ᮡḰᴦ≮ߢߪᚻⴚએᄖߩㆬᛯ
⢇߇ήߊ‫ޔ‬ᴦ≮ᓟߩ QOL ૐਅ߇⪺ߒ޿ߣ⠨߃ࠄࠇࠆ‫(ޔ‬2)PS҇2‫(ޔ‬3)㆙㓒ォ⒖ࠍ⹺߼ߥ޿‫੍߽ߡ߼⹺ߪߚ߹ޔ‬ᓟߦᄢ߈ߊ㑐ਈߒߥ޿‫(ޔ‬4)18F㧙BPA PET ᬌᩏߦߡ⣲≌/ᱜᏱ⚵❱㓸ⓍᲧ߇ 2.5 એ਄‫(ޔ‬5)ᢥ┨ߢหᴦ≮ᴺߦߟ޿ߡหᗧ߇ᓧࠄࠇߚ‫᧦ߡߴߔߩޔ‬ઙࠍḩߚߒߚ㗡㗪ㇱ≸ 13 ଀ߢ޽ࠆ‫ޕ‬ᕈ೎ߪ↵ᕈ 8 ଀࡮ᅚᕈ 5 ଀‫ޔ‬ᐕ㦂ߪ 39
ᱦ߆ࠄ 74 ᱦ㧔ᐔဋ 59㧕ߢ޽ߞߚ‫ޕ‬⚵❱ဳߪ⣼᭽ྙ⢩≸ 4 ଀‫ޔ‬ᖡᕈ㤥⦡⣲ 4଀‫ޔ‬ᚳᐔ਄⊹≸ 3 ଀‫੃ޔ‬㗡⁁⣼≸ 1 ଀‫ޔ‬⣼≸ 1 ଀ߢ޽ߞߚ‫ⷰߩ଀∝ోޕ‬ኤᦼ㑆ߪ‫ޔ‬6-17
ࡩ᦬(ᐔဋ 11.3)ߢ޽ߞߚ‫ޕ‬㻙㻌 㻟㻣㻥㻌㻙

JAEA-Review 2011-050

ᾖ኿ᣇᴺߪᾖ኿೨ߦ∛ᄌㇱࠍ↹௝(CT ߹ߚߪ MRI)᠟ᓇߒߚ߽ߩࠍ‫ޔ‬BNCT ኾ↪ᴦ≮⸘↹࠰ࡈ࠻ࠍ↪޿ߡ⹏ଔߒ‫✢⤏⊹ޔ‬㊂߇
15Gy-Eq‫✢⃿⌒ޔ‬㊂߇ 10Gy-Eq ࠍ⿥߃ߥ޿▸࿐ߢ⣲≌ᦨૐ✢㊂ࠍ 20Gy-Eq એ਄ߣߒߚ‫ޕ‬ᾖ኿ᣣߦ BPA500mg/kg ࠍ 3 ᤨ㑆߆ߌߡὐṢ㕒ᵈࠍⴕ޿‫⋥ੌ⚳ޔ‬ᓟߦᾖ኿૕૏ߩ࠮
࠶࠹ࠖࡦࠣᓟ‫ޔ‬ᾖ኿⋥೨ߦⴊਛࡎ࠙⚛Ớᐲࠍ᷹ቯߒߚ‫⋥ޕ‬೨ࡎ࠙⚛Ớᐲߣ‫ޔ‬15 ಽ㑆ߩਛᕈሶ✢㊂߆ࠄᦨ⚳⊛ߥᾖ኿ᤨ㑆ࠍ᳿ቯߒߚ‫ޕ‬〯 ߹ ߃ ᚒ ‫ ߪ ޘ‬BNCT ࠍ 㗡 㗪 ㇱ ≸ ᴦ ≮ ߩ
Neoadjuvant therapy ߣߒߡᴦ≮ࠍⴕ߁ߎߣ߇น⢻ߢ‫ޔ‬ᚒ‫ߪޘ‬ᒰᄢቇ୶ℂᆔຬળᛚ⹺
ߩ߽ߣ‫ޔ‬㗡㗪ㇱ≸ߩೋᦼᴦ≮ߣߒߡ BNCTࠍⴕߞߡ޿ࠆ‫⃻ޕ‬࿷ 3 ଀(2007 ᐕߩ 2 ଀ࠍ฽߻)ߩㅴⴕ㗡㗪ㇱ≸ߦኻߒߡᧄᴦ≮ࠍೋᦼᴦ≮ߣߒߡⴕ޿‫ޔ‬3 ଀ߩᐔဋⷰኤᦼ㑆߇18 ࡩ᦬ࠍ⿧߃ߚ⃻࿷ߢ߽‫଀ోޔ‬ή∛↢ሽਛߢ޽ࠆ‫੹ޕ‬ᓟ߽ߘߩᴦ≮ലᨐࠍᬌ⸛ߔࠆ੍
ቯߢ޽ࠆ‫ޕ‬㧔㧟㧕⚿ᨐ
ో 13 ∝଀ߩᴦ≮ലᨐߪ‫ޔ‬CR㧦8 ଀‫ޔ‬PR㧦
4 ଀‫ޔ‬NC㧦1 ଀ߢ޽ࠅ‫ޔ‬ᄼഞ₸ߪ 92.3㧑ߢ޽ߞߚ‫↢ޕ‬ሽ଀ 8 ଀ߩ⃻࿷߹ߢߩᐔဋⷰኤ
ᦼ㑆ߪ 14.8 ࡩ᦬ߢ޽ߞߚ‫ޕ‬ᱫ੢ߪ 5 ଀ߢ޽ߞߚ‫ޕ‬ᱫ੢଀ߩౝ⸶ߪ‫∛⃻ޔ‬ᱫ 4 ଀‫ઁޔ‬࿃
ᱫ 1 ଀ߢ޽ࠅ‫ޔ‬ᐔဋ↢ሽᦼ㑆ߪ 5.8 ࡩ᦬ߢ޽ߞߚ‫ޕ‬
ᾖ኿ߦ઻߁ GradeII એ਄ߩว૬∝ߪ⹺߼ࠄࠇߕ‫ߩઁߩߘޔ‬ว૬∝߽⹺߼ࠄࠇߥ߆ߞ
ߚ‫⃻ޕ‬࿷ߩߣߎࠈ᥅ᦼ᡼኿✢ว૬∝ߪ⹺߼ࠄࠇߡ޿ߥ޿‫ޕ‬㧔㧠㧕⠨ኤߣ߹ߣ߼
ᮡḰߩ㗡㗪ㇱ≸ᴦ≮ߢ೙ᓮਇน⢻ߥ∝଀ߦኻߒߡⴕߞߚᧄᴦ≮ߢߪ‫ޔ‬ᄼഞ₸ 92.3㧑
ߣ㕖Ᏹߦ㜞޿߽ߩߢ޽ߞߚ‫ޔߒ߆ߒޕ‬ㅴⴕ߅ࠃ߮ౣ⊒≸ߩ႐วߪ‫ޔ‬᣿ࠄ߆ߥ∛ᄌએᄖߦォ⒖߇㓝ࠇߡ޿ࠆ੐߇ุቯߢ߈ߕ‫ޔ‬ᚒ‫ޘ‬ߩ∝଀ߢ߽ẜ࿷∛ᄌ߇੍ᓟࠍᄢ߈ߊᏀฝߒ
ߚ‫ޔࠄ߇ߥߒ߆ߒޕ‬ౣ⊒∛ᄌߦኻߔࠆੑᰴ
ᴦ≮ߣߒߡߩ᦭ലᕈߪᚒ‫ᦨߩޘ‬ೋߩ∝଀ 3)߿ᧄ⚿ᨐ߆ࠄ᣿ࠄ߆ߢ޽ࠅ‫ޔ‬ട⮮ࠄ߽ߘߩ᦭ലᕈࠍ㜞ߊ⹏ଔߒߡ޿ࠆ 4)‫⚿ߩߘޕ‬ᨐࠍ

ෳ⠨ᢥ₂
1)Y,
Mishima.
Neutroncapturetreatment of malignant melanoma using
10B-chlorpromazine. Pigment Cell Res.
1:215-221,1973
2)Y Imahori, S Ueda, Y Ohmori, T
Kusuki, K Ono, R Fujii and T Ido.
Fluorine-18-labeledfluoroboronophenylalanine
PETinpatients
withglioma.
J.
Nucl.
Med.39:325-333,1998
3)Teruhito Aihara, Junichi Hiratsuka,
Norimasa Morita, et al 㧦 First clinicalcase of boron neutron capture therapy forhead and neck malignancies utilizing
18F-BPA PET. Head and Neck.-DOI 10
850-855 2006
4) I Kato, K Ono, Y Sakurai, M Ohmae,
A Maruhashi, Y Imahori, M Kirihata, M
Nakazawa and Y Yura. Effectiveness of
BNCT for recurrent head and neckmalignancies. Applied Radiation and
Isotopes 61:1069-1073,2004

5-1
ේሶἹ㧦JRR-4

ⵝ ⟎㧦BNCT ක≮ᾖ኿ⵝ⟎㻙㻌 㻟㻤㻜㻌㻙

ಽ ㊁㧦ߘߩઁ(⥃ᐥකቇ)

JAEA-Review 2011-050

5-2ș⥺᳨ฟ NMR-ON ࡟ࡼࡿ᰾≀ᛶࡢ◊✲
Study of Hyperfine Interaction using șray detected NMR-ON኱▮ 㐍㸪኱ᆤ 㝯㸪Ἠᕝ༟ྖ㸯㸪Ṋ⸨ ㇦㸰㸪すᮧඞᙪ㸱
S. Ohya,T. Ohtsubo, T. Izumikawa, S. Muto, K. Nisimura᪂₲኱Ꮫ⮬↛⛉Ꮫ◊✲⛉
Graduate School of Science and Technology, Niigata University㸯㸯᪂₲኱Ꮫ࢔࢖ࢯࢺ࣮ࣉ⥲ྜࢭࣥࢱ࣮

Radioisotope Center, Niigata University㸰㧗࢚ࢿࣝࢠ࣮ຍ㏿ჾ◊✲ᶵᵓ୰ᛶᏊ◊✲ᡤ㸰

Neutron Science Laboratory, KEK㸱ᐩᒣ኱ᏛᕤᏛ㒊㸱

Faculty of Engineering, Toyama Universityࡑࡇ࡛ࡇࢀࡽࡢၥ㢟ࢆゎỴࡍࡿࡓࡵᩘᖺ

㸯㸬ࡣࡌࡵ࡟ ᡃࠎ᪂₲኱Ꮫప๓࠿ࡽș᳨ฟჾࢆ +H+H ᕼ㔘෭෾ᶵࡢෆ㒊᰾ᩚิࢢ࣮ࣝࣉࡣࡇࢀࡲ

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ᡭἲࡣపᐃࡀᅔ㞴࡛࠶ࡗࡓ㉸ᚤ⣽┦஫స⏝ࢆș⥺ᨺฟ᰾ࡢ 10521 ࡢ᪉ἲ࡛◊✲ࡍࡿ㸬᰾೫ᴟ࠿ࡽࡢȚ⥺ࡢ␗᪉ᛶࡢᔂࢀ

ᮏᐇ㦂࡛ࡣ )H ࡢࢽࢵࢣࣝ୰ࡢ 10521 ࢆࢆ᳨ฟࡋ࡚᰾☢Ẽඹ㬆ࢆᚓࡿࡇ࡜࡛࠶ࡗࡓࠋ

⾜࠸ࠊඹ㬆ࡢほ㸪⦆࿴᫬㛫ࡢᐃ࡟ᡂຌࡋȚ⥺ࡣ +H+H ᕼ㔘෭෾ᶵࡢእഃ࠿ࡽ᳨ฟ࡛

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JAEA-Review 2011-050

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JAEA-Review 2011-050

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5-2

JAEA-Review 2011-050

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5-3

JAEA-Review 2011-050

5-3ਛᕈሶ᝝ᝒ≮ᴺߩ㔍ᴦᕈ≸ᴦ≮߳ߩㆡᔕ᜛ᄢߦ㑐ߔࠆၮ␆⊛࡮⥃ᐥ⊛⎇ⓥ
Basic & Clinical Research for Application of Neutron Capture Therapy
to Highly Advanced Cancerz

Measurement of Boron in Tumours by Neutron Capture Autoradiography following
intra-arterial Administration of Boron Entrapped Water-in-Oil-in-Water Emulsion
Yanagie Hironobu1,2, Mikado Shoji3, Yasuda Nakahiro4, Higashi Syushi5,
Ikushima Ichiro5, Mizumachi Ryuji6, Murata Yuji6, Morishita Yasuyuki7,
Shinohara Atsuko8, Ogura Koichi3, Sugiyama Hirotaka2,
Ryohei Nishimura9,Takamoto Sinichi2,10, Eriguchi Masazumi2,11,
and Takahashi Hiroyuki1,2

1Department of Nuclear Engineering & Management, Graduate School of Engineering,

The University of Tokyo,Tokyo, JAPAN, 2Cooperative Unit of Medicine & Engineering,
The University of Tokyo Hospital, Tokyo, JAPAN, 3Department of Physics, College ofIndustrial Technology, Nihon University, Chiba, JAPAN, 4Department of Physics,
National Institute of Radiological Sciences, Chiba, JAPAN,
5Miyakonojyo Metropolitan Hospital, Miyazaki, JAPAN, 6Department of Pharmacology,

Kumamoto Institute Branch, Mitsubishi Chemical Safety Institute Ltd, Kumamoto,JAPAN, 7Department of Human & Molecular Pathology, Graduate School of Medicine,
The University of Tokyo, Tokyo, JAPAN, 8Department of Humanities, The Graduate
School of Seisen University, Tokyo, JAPAN, 9Department of Veternary Surgery, The
University of Tokyo Veternary Hospital, Tokyo, JAPAN, 10Department of Cardiac
Surgery, The University of Tokyo Hospital, Tokyo, JAPAN, 11Department ofMicrobiology, Syowa University School of Pharmaceutical Sciences, Tokyo, JAPAN
Corresponding Author: Hironobu Yanagie, MD, PhD ; TEL: +81-3-5800-9194 ;FAX: +81-3-5800-9195 ; E-mail: yanagie@n.t.u-tokyo.ac.jp

1.

Introduction

The cytotoxic effect of BNCT is due to a nuclear
reaction between 10B and thermal neutrons(10B + 1n o7Li + 4He + 2.31 MeV (93.7 %) /2.79 MeV (6.3 %)). The resultant lithium ionsand  particles on neutron capture reaction arehigh LET(linear energy transfer) particles withrelatively high biological efficiency.
These
particles (D and 7Li) destroy cells within about
10m path length from the site of the capture
reaction. It is theoretically possible to killtumour cells without affecting adjacent healthy
cells, if the former can selectively accumulate
10B atoms. So It is very important to develop
selective boron delivery systems for effective

JRR3, Thermal Neutron Irradiation Facility, Neutron Capture Autoradiography㻙㻌 㻟㻤㻡㻌㻙

JAEA-Review 2011-050

BNCT therapy (Yanagie, 1991, 1997, 2004,
2006a). BNCT has been used clinically inpatients with malignant brain tumours andmelanoma.
Liposomes
have
been
investigatedextensively as carriers for anticancer drugs inattempts to direct active agents to tumours or
to protect sensitive tissues from toxicity. We
have reported that 10B atoms delivered byimmunoliposomes are cytotoxic to humanpancreatic carcinoma cells (AsPC-1) afterthermal neutron irradiation in vitro(Yanagie,
1991).
The intra-tumoural injection ofboronated immunoliposomes can increase theretention of 10B atoms in tumour cells, causing
suppression of tumour growth in vivo following
thermal neutron irradiation (Yanagie, 1997).
We prepared polyethylene- glycol binding
liposomes (PEG-liposomes) as an effective 10B
carrier to obviate phagocytosis by RES.
Hepatocellular
carcinoma(HCC)
isdifficult to cure with operation, chemotherapy,
or radiation therapy. Iodized poppy-seed oil(IPSO) has a property of depositing itself
selectively in the cells of HCC, and theusefulness of iodized poppy-seed oil (IPSO) for
detecting or treating liver cancer was firstreported.
The oil has the property ofdepositing itself selectively in the cells of HCC.
Kanematsu et al. reported a method that mixed
a water-soluble antitumour agent with IPSO.
In their reports, an aqueous solution of an
anticancer drug, doxorubicin, was mixed with
60% urografin, a water-soluble contrast
medium, before the solution was mixed withthe oil (IPSO) (Kanematsu, 1989).
Higashi et al prepared a long term
inseparable, water-in-oil-in-water emulsion(WOW) containing 8-60 mg of epirubicin for use
in arterial injection therapy for patients withHCC (Figure 1) (Higashi, 1993, 1995).
Higashi et al had reported that tumour size of
HCC was reduced in six of seven patients, anda 50% or greater decrease of initialalpha-fetoprotein (AFP) levels within 14 days
was observed in all four patients who showedabnomal levels of serum AFP before treatment(Higashi, 1995).

According to the Higashi’s clinical results,
we would like to apply BNCT to treatment of
Hepatocellular Carcinoma (HCC) for increasing
the selection of therapies of HCC’s patients(Yanagie, 2006b). In this study, we develop
BSH entrapped WOW emulsion and evaluate
the emulsion as selective boron delivery carrier
to cancer tissues.
The accurate measurement of 10B
distributions in biological samples with asensitivity in the ppm range is essential forevaluating the potential usefulness of various
boron-containing compounds for BNCT.
We applied CR-39 (polyallyldiglycol
carbonate)plastic
track
detectors
toalpha-autoradiographic measurements of the
10B biodistribution in sliced whole body hepatic
samples of VX-2 tumour bearing rabbit. The
subsequent use of an alpha-track radiographic
image
analysis
systemenabledadiscrimination between alpha-tracks andrecoiled proton tracks was made by track size
selection method. This enabled to estimate
quantitatively the distributions of 10B
concentrations within the tissue sections
comparing using suitable standards (Yanagie,1999).

Figure 1. Microphotograph of WOW emulsion
In our study, we performed the neutron capture
autoradiography (NCAR) using CR-39 tracketch
detectors
toqualitatively
and
10B
quantitatively
determinethebiodistribution in hepatic samples of VX-2
tumours after intra-arterial injection of 10B
entrapped WOW emulsion.

5-3㻙㻌 㻟㻤㻢㻌㻙

JAEA-Review 2011-050

2.

Materials & Methods
Chemicals : Sodium salt of undecahydromercaptocloso-dodecaborate (Na210B12 H11 SH)
was obtained by Wako Chemical Co. Ltd.
(Tokyo, Japan). Iodized poppy-seed oil (IPSO,
Lipiodol Ultrafluid, Kodama, Co., Ltd., Tokyo,
Japan) is composed of iodized ethyl esters of
the fatty acids obtained from poppy-seed oil
and contains 37% iodine.

Preparation of Boron entrapped WOW
emulsion : Three hundred milligrams of BSH
was dissolved in 5 ml of a 5% glucose solution
and filtrated of controlled pore glass membraneemulsifying into 5 ml of IPSO containing
surfactant, to form the water-in-oil emulsion(WO).
The WO emulsion was thenemulsifyied again with aqueous phase
containing 5 ml of saline and surfactant. With
this double emulsifying technique, the BSH
entrapped WOW emulsion was prepared(Higashi, 1995, Yanagie, 2006b). The particle
size distributions of the vesicles of WOW andIPSO microdroplets were determined with alaser-diffraction
particle-size
analyzer
SALD-2000 (Shimadzu Corp., Kyoto, Japan).
The boron concentration entrapped in WOW
vesicles was determinated by ICP- Mass
Spectroscopy at Jyuntendo University.

the boron concentrations of the tumour nodules
and normal liver tissues were determinated bySpectroscopyatJyuntendo
ICP-Mass
University. (Yanagie, 1999).

Preparation of standard samples and sliced
mice samples : In order to examine thebiodistribution of the10

B entrapped WOW

emulsion after intra-arterial injections to thehepatic artery propria, we carried out
Neutron-Capture Auto Radiography(NCAR).
Rabbits were sacrificed 1 and 3 days after the
injection of

10

B-WOW emulsion, and thehepatic samples were frozen at -60 ͠ .
Subsequently, the frozen samples were cut
sagittally into 40 m thick sections mounted ona thin 3M Scotch tape, freeze-dried at -20͠ for
two weeks and air-dried for one more week.
Thus, the dried samples were prepared.
Boron-containing standard samples were also
prepared using drying filter paper sheets
wetted by BSH solutions of four different 10B
concentrations(10, 50, 100, 500 ppm of 10BSH),
respectively. The 10B concentrations of 10BSH
solutions were determined by ICP-Mass
Spectroscopy at Jyuntendo University.

Neutron irradiation : The sliced sections were
In vivo Experiments : VX-2 rabbit squamouscell carcinoma cell line was cultured in vitro
supplemented with of 10% fetal bovine serumand 500mg streptomycin/penicillin in 5% CO2
condition. The VX-2 cells were inocculated
onto the foot pad of the rabbits, and then, thetumours of VX-2 were formed after one week
feeding. The nodules of VX-2 tumour wereinocculated to left hepatic lobe of liver, then,the hepatic tumour models were constructed
after two weeks feedings.
After 2 weeks
tumour inocculation, BSH entrapped WOW
emulsionswereadministeredwith
intra-arterial injections via the hepatic artery
propria compared with 10BSH-Lipiodol mixed
conventional emulsion ( 10BSH : 75 mg/kg
rabbit) on VX-2 rabbit hepatic tumour models.
One and three days after arterial injections,put in close contact with the CR-39 plates(HARZLAS TD-1; Fukuvi Chemical Industry,
Japan) using thin adhesive tape. The set of
hepatic samples of VX-2 tumour bearing rabbit
were simultaneously exposed in the JRR3
reactor of Japan Atomic Energy ResearchInstitute.
The thermal neutron fluence
irradiation was varied according to theexperimental objectives.
For alpha track counting (i.e. 10B distribution
measurements) : 2.0 x 1010 n/cm2 .
For the visible observation of NCAR image:
2.0 x 1012 n/cm2 .

Etching procedure :For NCAR imaging
utilized- and Li tracks as well as protons ofrecoiled and/or produced by 14N (n, p) reaction,㻙㻌 㻟㻤㻣㻌㻙

JAEA-Review 2011-050

where 14N is the biogenically abundant nuclide,
the CR-39 detector plates were etched in a 7 N
NaOH solution at 70 ͠ for 2 hours to reveal
tracks.

3.

Table 1. 10B concentration of VX-2 hepatic
tumour bearing rabbit model
after intra-arterial injection of 10B-WOW
emulsion or 10B-Lipiodol mix

Results & Discussion

We prepared BSH entrapped WOW emulsion.
The mean 10B concentration was 13000 ppm by
ICP-MAS. The size of WOW was controlled to
50m.
The 10B concentration in VX-2 tumour was
141 ppm, 61 ppm by WOW emulsion after 1 day,or 3 day intra-arterial injection, respectively.
The 10B concentration of tumour was 58,
24ppm by Lipiodol mix emulsion after 1 day, or
3 day same injection, respectively (Table 1).
The histological staining showed thesuperior accumulation of the fat droplets ofWOW emulsion in tumour site compared with
Lipiodol mix emulsion.
Electromicroscopic
figure of hepatocellular carcinoma afterarterial- injection chemotherapy using WOW
emulsion : The microdroplets of Iodized
poppy-seed oil was retained in the cytoplasm of
the cancer cell in the same conformation as
preparation time, but there was noaccumulation of fat droplets in Lipiodol
emulsion. The 10B concentrations of samples
were determined by ICP-Mass Spectroscopy at
Juntendo University
From NCAR image of sliced samples, we
can estimate the 10B accumulations in theorgans. 10B accumulations were estimated forthe strongly concentrated part of the tumour atday 3 after injection by WOW emulsion. In
order to show the imaging of 10B accumulationin tumour, we obtained NCAR image of sliced
samples of VX-2 hepatic tissues using CR-39
track etch detector. NCAR image consists of alarge number of etch pits, such as proton, and Li tracks. The track area of the opening
mouth of each etch pit as well as its position
was analyzed by the automated digital imaging
optical microscope (HSP-1000), whose image
acquisition speed is 50-100 times faster thanconventional microscope system15). NCAR

WOW Tumour
Normal Liver Blood--------------------------------------------------------------------Day-1
141.8
6.1
1.2
Day-3
61.7
4.3
0.1
--------------------------------------------------------------------Lipiodol Tumour Normal Liver Blood--------------------------------------------------------------------Day-1
58.0
14.6
0.4
Day-3
24.5
3.9
0.2
---------------------------------------------------------------------

images of tumour in hepatic tissues are shownin Fig. 2. These images were reconstructed bymeans of scatter plots for the x-y coordinate of
the observed whole tracks. Each dot appearing
in Fig. 2 corresponds to tracks one by one.
Figure 2 shows NCAR of tumour or normalliver site of VX-2 hepatic tissues from a set of
VX-2 hepatic cancer bearing rabbit that havereceived intra-arterial injections of 150 mg of
10B by WOW emulsion or Lipiodol mix solution.
The slices of sacrificed and frozen sections wereprepared 3 days after injection. 
It is difficalt to assess 10B accumulationand distribution in the sample, because theimages of Fig. 2 were contaminated by proton
tracks. In order to know the efficiency of
intra-arterial boron delivery carrier for BNCT,
it is necessary to discriminate- tracks fromproton tracks. Generally, etch pit size of the
track in the plastic track detector depends on
the LET value of the incident particle. In thiscase, LET values for protons are less than 100
keV/Ǵm. The tracks with LET greater than
100keV/ Ǵ m are actually due to - and Li
particles from the10B(n, ) 7Li reaction and the
maximum values are 2.4 x102 keV/Ǵm and 3.9
x 102 keV/Ǵm, respectively16). Therefore, twopeaks of track size appear in the track area
distribution, the lower peak corresponds toproton tracks, and the higher one is due to and Li tracks. It is considered that the㻙㻌 㻟㻤㻤㻌㻙

5-3

JAEA-Review 2011-050

contribution of Li tracks is not so large becauseof the short range of Li particles. The track size
discrimination between- and proton tracks
has been done using observed track area
distribution and subtracted proton tracks from
Fig. 2. The results are shown in Fig. 3. The
distribution of -tracks was obtained, then weare able to recognize accurate 10B accumulationand distribution in the VX-2 tumours. It isreadily apparent that the-etch pit reveals theexistence of 10B atoms delivered by WOW
emulsion into the VX-2 tumour. Accurate 10B
accumulationin the VX-2 tumours wasachieved by WOW emulsion. When the 10B
Lipiodol mix solution was injected to thetumour bearing rabbit, the accumulation of 10B
atoms in the tumour was small. The-track
densities of normal liver is not detected at 3days after intra-aterial injection, so theclearance of WOW emulsion and Lipiodol mix
solution in the healthy tissue is very rapid.
The measurement of 10B distributions inbiological samples with a sensitivity in the ppm
range is essential for evaluating the potential
usefulnessofvariousboron-containing
10B accumulations incompounds for BNCT.
the tumour varies by boron delivery systems, so
we find the strong and weak, concentrated
parts of the tumour after injection (Yanagie,
1999. It is necessary to supply the boron
atoms homogeneously in the tumours for
effective BNCT.
The study of the
microdosimetry of 10B atoms is ongoing, andCR-39 radiography using track counting will bepossible to determine the micro- or finestructure, i.e. micro-autoradiography, of 10B
distribution in the tumour (Ogura, 2001).
Clinically,administrationofWOW
emulsion drug encapsulated anti-cancer
reagent in inner droplets, is surprisingly
effective for both terminal and multi-originatedin HCC when the drug is injected to suffered
liver through a catheter inserted in liver artery.
10B entrapped WOW emulsion is possible todeliver and transport the boron atoms to thecancer cell in tumour tissues. These results
have shown that 10B entrapped WOW emulsion
is most useful for intra-arterial boron delivery

carrier on BNCT to cancer. We now plan invivo evaluation of 10B entrapped WOW
emulsion, and the clinical trial of BNCT for
HCC patients, and hope to perform first BNCT
trial with WOW emulsion in near future.

10B-WOW emulsion

Normal Liver

Tumor

10B-Lipiodol Mix solution

Tumor

Normal Liver

Figure 2 . Alpha and proton track etch pits
distributions of the tumour after 3 days
injection of 10B entrapped WOW emulsion(Left) / 10B Lipiodol mix solution (Right) on
VX-2 hepatic tumour bearing rabbit. This
image shows tumour or normal liver site of aneutron-capture radiograph from a set of VX-2
hepatic cancers bearing rabbit that havereceived intra-arterial injection of 150 mg of
10B. The slices of sacrificed and frozen tissues
were prepared 3 days after injection.

4.

Conclusion

We will be able to apply boron entrapped WOW
emulsion to BNCT for hepatocellular
carcinoma, and NCAR technique for detection5-3㻙㻌 㻟㻤㻥㻌㻙

JAEA-Review 2011-050

of effective 10B carrier in BNCT for cancer.
10B-WOW emulsion

Normal Liver

Tumor

10B-Lipiodol Mix solution

Tumor

Normal Liver

Figure 3. 10B distributions of the tumour after 3
days injection of 10B entrapped WOW emulsion(Left) / 10B Lipiodol mix solution (Right) on
VX-2 hepatic tumour bearing rabbit. Images
were obtained by the subtraction of proton
track data from Fig. 2.

Autoradiography
following
intra-arterial
Administration of Boron Entrapped Water-inOil-in-Water
Emulsion.
Proc.
of
13th
International Congress of Neutron Capture
Therapy, pp713-718.
Mikado S., Yanagie.H, et al. 2008. Applicationof Neutron Capture Autoradiography to Boron
Delivery Seeking Techniques for Selective
Accumulation of Boron Compounds to Tumorwith Intrarterial Administration of Boron
Entrapped Water-in-oil-in-water Emulsion.
NIMA inpress.
Yanagie H, et al. 2006. Selective Enhancementof Boron Accumulation with Boron-Entrapped
Water-in-oil-in-water Emulsion in VX-2 Rabbit
Hepatic Cancer Model for BNCT. Proc. of 12th
International Congress of Neutron Capture
Therapy, pp211-214.
Amemiya H., yanagie H., et al. 2005.
High-resolution nuclear track mapping indetailed cellular histology using CR-39 withtechnique.
thecontact
microscopy
RadiationMeasurements, 40,
Issues2-6,
283-288.

Acknowledgements
This work was supported in part by aGrant-in-Aid from the Ministry of Education,
Science and Culture, Japan (No. 11691202 andNo. 11557092 to Hironobu Yanagie).
Thethermal neutron irradiation was carried out
using the JAEA (Tokai) JRR3 facility supportedby the Inter-University Program for the Joint
Use of JAEA Facilities.

5. Publications
Yanagie. H, et al. 2008. Measurement of Boronby
NeutronCapturein
Tumours5-3

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JAEA-Review 2011-050

5-4ਛᕈሶ᝝ᝒ≮ᴺߩ㔍ᴦᕈ≸ᴦ≮߳ߩㆡᔕ᜛ᄢߦ㑐ߔࠆၮ␆⊛࡮⥃ᐥ⊛⎇ⓥ
Basic & Clinical Research for Application of Neutron Capture Therapy
to Highly Advanced CancerzInhibition of Tumor Growth of Mouse Colon Cancer Cell Line by Boron Neutron
Capture Therapy & ImmunotherapyzFeasible Evaluation of Neutron Capture Therapy for Local Recurrenced Breast
CancerH. Yanagie1 ,2, K. Kakimi2,3, A. Hosoi2,3, A. Ogata2, K. Mouri2, K. Eguchi2, Y. Morishita4,
A. Shinohara5, H. Kumada6, T. Nakamura6, Y. Furuya7, S. Takamoto2,8,
M. Eriguchi2,9, and H. Takahashi1,21Department of Nuclear Engineering & Management, Graduate School of Engineering,

The University of Tokyo, 2 Cooperative Unit of Medicine & Engineering, The Universityof Tokyo Hospital, 3Department of Immunotherapeutics (Medinet), The University ofTokyo Hospital, 4Department of Human & Molecular Pathology, Graduate School of
Medicine, The University of Tokyo, 5Department of Hygenes, School of Medicine,
Jyuntendo University, Tokyo, 6Japan Atomic Research Institute, Ibaraki, 7Departmentof Surgery, Satukidai Hospital, Chiba, 8Department of Cardiac Surgery, The Universityof Tokyo Hospital, Tokyo, 9Department of Microbiology, Syowa University School of
Pharmaceutical Sciences, Tokyo, JAPAN
Corresponding Author: Hironobu Yanagie, MD, PhD ; TEL: +81-3-5800-9194 ;FAX: +81-3-5800-9195 ; E-mail: yanagie@n.t.u-tokyo.ac.jp
1. Introdeuction
The cytotoxic effect of BNCT is due to a nuclear
reaction between 10B and thermal neutrons (10B +1
n o7Li + 4He + 2.31 MeV (93.7 %) / 2.79 MeV(6.3 %)). The resultant lithium ions and D
particles are high linear energy transfer (LET)
particles which give important biological effect.
Their short range in tissue (5 - 9 Pm) restricts
radiation damage to those cells in which boron
atoms are located at the time of neutron
irradiation.
Liposomes can contain a large amount of 10B

compound, which can be delivered to tumor cells.
We have reported that 10B atoms delivered byimmunoliposomes are cytotoxic to humanpancreatic carcinoma cells (AsPC-1) with thermal
neutron irradiation in vitro (Yanagie, 1991), andintratumouralinjectionofboronated
immunoliposomes can increase the retention of 10B
atoms in tumour cells, and suppress tumour
growth in vivo under thermal neutron irradiation(Yanagie, 1997).
Dendritic Cells (DCs) are potent antigenpresenting cells that can both activate innate andacquired immune responses, so it is now being
focused on the role of DCs in eliciting antitumor

JRR4, Thermal Neutron Irradiation Facility of Reactor, JCDS, BNCT㻙㻌 㻟㻥㻝㻌㻙

JAEA-Review 2011-050

immunity and in potential therapeutic applications.
For example, administration of DCs loaded ex vivo
with tumor-associated antigens can elicit antitumor
immunity resulting in tumor regression in various
murine tumor models, and DCs pulsed with tumor
derived peptides, proteins, genes or tumor lysates,
as well as DCs fused with tumor cells, have all beenstudied as therapeutic cancer vaccines (Chang,2002). Candido et al had reported that theyevaluated the effect of IT injections of bonemarrow derived DCs on the subcutaneous growthof the murine MT-901 breast tumor (Candido,2001). They demonstrate that DCs can efficiently
uptake apoptotic MT-901 tumor cells and that local
injections of DCs alone can result in regression ofthis breast tumor in vivo, which is dependent onhost CD8 T-cell immunity.
Recently, it has been reported that combined
immuno and radiation therapy results in effective
tumor growth suppression. Radiation therapy iscurrently applied in the treatment of a wide arrayof human cancers. Recent evidence indicates thatbesides exerting direct toxic effects on tumor cells,
ionizing
radiation
also
exhibits
variousimmunomodulatory  effects.  Inflammatory
responses are triggered within irradiated tissues
recruiting DCs to sites of inflammation. At the site,
DCs acquire antigens, undergo maturation, andthen migrate to the draining lymph node, where
they present processed antigens to T cells.
Irradiated tumor cells have been shown to serve
effectively as a source of  Tumor Associated
Antigens (TAAs) to elicit specific T-cell responses
in vitro when processed and presented by DCs(Strome, 2002).
We would like to apply BNCT, toradioresistant conditions as recurring &advancedbreastcancer,hepatocellular
carcinoma, liver metastases, or lung cancer.
Incidence of breast cancers is increasing, so it isalso more important to plan treatment
protocols for recurring cases (Ballo, 1999, Liao,
2000). Breast cancer may recur after primary
resection both locally (thoracic wall :23%, local
lymph nodes :19%) and in distant sites(bone :23%, lung : 18%, and liver : 4%). The
treatment of local recurrences may be curative
or palliative to avoid the occurrence of

bleeding, ulcer formations, bad smelling.
Radiation therapy is commonly used to thispurpose (Nielsen, 2006, Touboul, 1999, Willner,
1997). Skin ulcer, and bone necrosis may
apper after irradiation due to the lower
tolerance of the thoracic wall after mastectomy.
So a dose of about 40~50 Gy is recommended
for recurrences.
In our study, we prepared the cationicliposome (COATSOME-EL) as the effective 10B
carrier to deliver the boron atomes into the cancer
cells as the manner of gene delivery systems, andwe evaluated the synergic anti-cancer effects ofimmune-responces
withdendritic
cells
intratumoral injection after BNCT.
We also evaluate neutron flux dosimetry inhorizontal irradiation position using a phantom
a mammary gland at Kyoto
model of
University Research Reactor, and also evaluate
the BNCT simulation for a breast cancer
patient with MRI images using JCDS at Japan
Atomic Energy Research Institute.

2. Materials & Methods
Chemicals : Sodium salt of undecahydromercaptocloso-dodecaborate (Na210B12 H11 SH) was
obtained by Wako Chemical Co. Ltd. (Tokyo,
Japan).
Preparation of Liposomes containing 10BCompound : A cationic empty liposome(COATSOME EL-C-01 : Nichiyu liposome Co.
Ltd.)
iscomposedwith
L-a-dipalmitoyl
phosphatidylcholine (26 moles), cholesterol (20moles), and stealylamine (4 moles).
BSH(10mg/ml) solution was added to the COATSOME
EL-C-01, and made the 10B-liposome solution(Yanagie, 1999).
The boron concentration
entrapped in COATSOME-EL vesicles wasdeterminated by ICP- Masspectroscopy of
Jyuntendo University.
Generation of Bone Marrow-Derived DCs : Bonemarrow cells obtained from femurs and tibias of
BALB/c mice were cultured in RPMI 1640 medium
supplemented with 10% FCS, 12.5 mM HEPES, 5

㻙㻌 㻟㻥㻞㻌㻙

5-4

JAEA-Review 2011-050

x 10-5 M 2-mercaptoethanol, 1 x 10-5 M sodium
pyruvate,
1%
NEAA,
10
mg/ml
Penicillin/Streptomycin and 20 ng/ml GM-CSF(PeproTech, Rocky Hill, NJ) for 7 days. On day 7,
DCs were harvested by gentle pippetting, washedtwice with PBS and resuspended at 1 x 107 cells/0.1
ml PBS for intratumoral injection (Saji, 2006).

in the absence or presence of irradiated (60 Gy)
Colon26 tumor cells (5 x 103 cells in 100 l of CM).
The assays were performed and developed using
anti-mouse IFN-mAb according to the kit
manufacturer’s instructions (BD Pharmingen).
All experiments were performed in duplicate andthe data correspond to the mean value.

Splenocytes : Spleen cells,
harvested from
BALB/c mice, were treated  with ammonium
chloride-potassium lysis buffer (0.83% ammonium
chloride, 0.1% KHCO3, and 0.004% EDTA) for
5 min to deplete erythrocytes and washed twicewith HBSS. They were then enumerated andresuspended in HBSS for injection (Saji, 2006).

Adoptive Transfer Model. : Splenocytes harvested
from treated mice on day 40 after tumor
inoculation were transferred intraveneously tosyngeneic mice.
Two days after spleen cells
transfer, Colon26 cells (5 x 105 cells) were injectedsubcutaneously.
The effect of anti-tumor
immunity was evaluated on the basis of tumor
volume (Saji, 2006).

BNCT procedure : The Colon26 (1 x 106) cells were
injected subcutaneously into the back of the male
BALB/C mice (Nihon SLC). Ten days after
injection, when an average diameter of 10 mm wasreached , 150 l of
injected(IT).

Animal Etics : The procedures for the tumor
implantation and the sacrifice of the animals werein accordance with approved guidelines of theInstitution’s Animal Ethics Committee.

10

B-liposome solution were
10

The mice injected with B-liposome

solutions were irradiated with thermal neutrons (2x 1012 n/cm2) at JRR4 reactor of Japan Atomic
Energy Research Institute.
DC treatment : On day 10, when the tumors
reached an average diameter of 10 mm, BNCT on
mice IT injected with 10B entrapped liposome was
performed and, at thatᴾ time,
syngeneic DCs(1 x 107 cells/mouse) were injected
IT with the schedule 1 (day 0, day 3 , day 6), or
schedule 2 (day 0, day 3, day 6, day9, day 12, day
15, day 18). After BNCT+DCs injections, theeffect of treatment was calculated on the basis oftumor volume and morphological findings of thetumors at 4-day intervals.
ELISPOT Assay. : Tumor-specific T cell responses
wereevaluatedby
ELISPOT
assays.
Erythrocyte-depleted splenocytes harvested fromtreated or control mice 40 days after tumor
inoculation or from age matched naive mice (5 x
104 splenocytes in 100 l of CM) were placed into
each well and incubated for 24 h at 37°C, 5% CO2

Neutron dosimetry with JAERI Computational
Dosimetry System (JCDS) for a breast cancer
patient: : BNCT was simulated in a 64 years
patient with a 3 cm tumour in the lower half of
the R breast. LiF collimation was used to
selectively irradiate the tumor while sparing
the adjacent normal organs (lung, heart). The
Neutron Beam Facility at JRR4 enables tocarry out boron neutron capture therapy withThe JAERI
epithermal neutron beam.
Computational Dosimetry System (JCDS),
which can estimate distributions of radiation
doses in a patient’s head by simulating in orderto support the treatment planning forepithermal neutron beam BNCT, wasdeveloped.
We applied this JCDS for
evaluation the neutron dosimetry for this case.

3. Results & Discussion
In order to evaluate that local BNCT followed byᴾ
IT-DC can inhibit primary tumor growth, BALB/cmice wereᴾ injected s.c. with Colon26 tumor cells.
On day 10, the tumors reached an average
diameter of 10 mm, BNCT on IT with 10B
entrapped liposome was done at thatᴾ time and5-4㻙㻌 㻟㻥㻟㻌㻙

JAEA-Review 2011-050

mice (Figure 3).
㪙㪥㪚㪫䈫㪛㪚ᵈ኿䈱૬↪ലᨐ䋨㪺㫆㫃㫆㫅㪄㪉㪍䇮㪉㪇㪇㪎㪅㪌㪅㪉㪌䉋䉍䋩
㪐㪇㪇㪇

㪏㪇㪇㪇

㪎㪇㪇㪇

㫍㫆㫃㫌㫄㪼㩿㫄㫄㪊㪀

㪍㪇㪇㪇

㪌㪇㪇㪇

㫅㫆㫅㪄㫋㫉㪼㪸㫋㪛㪚㪙㪥㪚㪫㪙㪥㪚㪫㪂㪛㪚

㪋㪇㪇㪇

㪊㪇㪇㪇

㪉㪇㪇㪇

㪈㪇㪇㪇

㪇
㪈㪉

㪈㪎

㪉㪉

㪉㪎
㪻㪸㫐

㪊㪉

㪊㪎

㪋㪉

Figure 1. Effect of combination treatment with
BNCT and IT-DC on Colon26ᴾ tumors.
㪙㪥㪚㪫䈫㪛㪚ᵈ኿䈱૬↪ലᨐ䋨㪺㫆㫃㫆㫅㪄㪉㪍䇮㪉㪇㪇㪎㪅㪍㪅㪏䉋䉍䇮⣲≌૕Ⓧᄌൻ䋩
㪈㪋㪇㪇㪇

㪈㪉㪇㪇㪇

㪈㪇㪇㪇㪇

㫍㫆㫃㫌㫄㪼㩿㫄㫄㪊㪀syngeneic DCs were injected intratumorally withthe schedule 1 (day 0, day 3 , day 6), or schedule 2(day 0, day 3, day 6, day9, day 12, day 15, day 18).
On schedule 1, although the tumors grew rapidly
following treatment with saline alone, and IT-DC,
the group treated BNCT + IT-saline and the
combination of BNCT + IT-DC ᴾ resulted insignificant suppression of tumor growth (Figure 1).
Almost all animals treated with BNCT + It-saline,
and BNCT + IT-DC became tumor-free. On
schedule 2, 30% tumor growth suppression wasachieved on IT-DC group, and also the grouptreated BNCT + IT-saline, and the combination of
BNCT + IT-DCᴾ resulted in significant suppressionof tumor growth compared to non-treated group(Figure 2).
Because both components of the combined
treatment, BNCT+DC, are delivered directly tothe tumor, we investigated whether thisprotocol could induce a systemic antitumor
response. It has been reported that in vitro
tumor-specific IFN-production by host-derived
T cells correlated with systemic antitumor
immunity in vivo. We evaluated whether
treatment of Colon26 tumor-bearing mice with
BNCT+DCs
could
elicittumor-specific
IFN-secreting T cells using ELISPOT assays .
Splenocytes retrieved on day 40 after tumor
inoculation from mice subjected to the BNCT+
3 times DCs combined therapy showedslightlyactivatedtumor-specific
IFN--secreting cells, while schedule 2 with
BNCT+ 7 times DCs resulted in significantly
more tumor-specific IFN--secreting cells
compared with splenocytes from control groups(data not shown).
To examine whether tumor-specificimmune response was induced in BNCT-DC
treated mice, splenocytes harvested fromtreated mice on day 40 after tumor inoculation
were transferred i.v. to syngeneic mice, and,Colon26 cells (5 x 105 cells) were injectedsubcutaneously. In tumor challenged mice,that received spleen cells from DC-treated mice
and BNCT-treated mice, tumor growth was
suppressed by 25%. Fifty % reduction intumor growth was observed in mice thatreceived spleen cells from BNCT+DCs treated㪏㪇㪇㪇㫅㫆㫅㪄㫋㫉㪼㪸㫋㪛㪚㪙㪥㪚㪫㪙㪥㪚㪫㪂㪛㪚

㪍㪇㪇㪇

㪋㪇㪇㪇

㪉㪇㪇㪇

㪇
㪈㪉

㪈㪎

㪉㪉

㪉㪎

㪊㪉

㪊㪎

㪋㪉

㪋㪎

㪻㪸㫐

Figure 2. Enhancement of tumor growth
suppression with increased intratumoral
injections of DCs on BNCT and IT-DC
treatments.
Celluzzi et al. had reported that it is possiblethat radiation augments the antitumor efficacy
of DC administration by modifying tumor cells
to become more immunogenic (Celluzzi, 1998).
This would allow ex vivo-generated functional
DCs to acquire TAAs from irradiated tumor
cells more efficiently than they would acquirethem from nonirradiated tumor cells. One of
the hallmarks of inflammation is an increase in
the permeability of the local vasculature that
leads to recruitment of circulating leukocytes
into surrounding tissues. Recently, it has
been shown that necrotic tumor cells can serve
as a source of multiple TAAs to pulse DCs as
effectively as apoptotic tumor cells (Kotera,
2001). Radiation has been reported to induce

5-4㻙㻌 㻟㻥㻠㻌㻙

JAEA-Review 2011-050

cytokines, chemokines, and inflammatory
mediator release and to upregulate theexpressionofadhesionmolecules,
co-stimulatory molecules, and heat shockproteins in tumor, stromal, and endothelial(Friedman,2002).
Thus,
the
cells
proinflammatory microenvironment within
irradiated tumors could provide DCs withmaturation-inducing
stimulicriticalfor
elicitingeffective
antigenpresentation.
Radiation facilitates the extravasation of bothantigen-presenting cells (Nikitina, 2001) andeffector T cells (Quarmby, 1999) into solid
tumors.
㪙㪥㪚㪫䈫㪛㪚ᵈ኿䈱૬↪ലᨐ䋨㪺㫆㫃㫆㫅㪄㪉㪍䇮㪉㪇㪇㪎㪅㪎㪅㪐䉋䉍䇮⣲≌૕Ⓧᄌൻ䋩
㪊㪌㪇㪇

㪊㪇㪇㪇

㫍㫆㫃㫌㫄㪼㩿㫄㫄㪊㪀

㪉㪌㪇㪇

㪉㪇㪇㪇

㫅㫆㫅㪄㫋㫉㪼㪸㫋
㪛㪚
㪙㪥㪚㪫

㪈㪌㪇㪇

㪙㪥㪚㪫㪂㪛㪚

㪈㪇㪇㪇

㪌㪇㪇

㪇
㪊

㪏

㪈㪊

㪈㪏

㪉㪊

㪉㪏

㪊㪊

㪊㪏

㪻㪸㫐

Figure 3. Tumor growth suppression with adoptive
immunity by BNCT+DCs on new challenging
Colon26 tumor
In these experiments, our data indicatethat DC administration combined with BNCT
cellularinduces
tumor
antigen-specificmediated immune responses in tumor bearing
mice. DCs combined with BNCT of a solitary
tumor confers protection against tumor
rechallenge. It is thought that tumor antigens
derived from necrosis, apoptosis, andinflammation induced by BNCT had beenpresented to DCs in BNCT+DCs combined
therapy. The growth of Colon26 tumors was
highly suppressed in mice that received
splenocytes from BNCT+DCs treated mice.
Regulatory T cells and suppressor macrophage
will be necessary to delete in the adoptive
splenocytesformore
stimulation
theanti-tumor immunity (not clear). We hope toapply this direct DC immunotherapy forenhancing the BNCT effects in clinical trials.
Kumada et al had reported that JCDS is a
software that creates a 3-dimensional headmodel of a patient by using CT scan and MRI
images, and that generates a input data fileautomatically calculation of neutron flux andgamma-ray dose distributions in the brain with
the Monte Carlo code MCNP, and that displaysthese dose distributions on the head model for
dosimetry by using the MCNP calculation
JCDS has theresults (Kumada, 2001).
following advantages; (1) a detailed 3D modelof the patient’s head can be easily obtained
from the CT and MRI data, (2) the
three-dimensional head image is editable tosimulate the state of a head after surgery, (3)JCDS can provide information for the Patient
Setting System which can support to set thepatient to an actual irradiation position swiftly
and accurately.
We performed the dosimetry with JCDS in
the condition of BNCT using epithermal
neutron beams(Figure 4). To decrease theskin side effects, the skinRBE dose limited to
10Gy-Eq. The minimum tumor RBE dose is
11.3 Gy-Eq, the mean tumor RBE dose is 28.9
Gy-Eq, and the maximum tumor RBE dose isThe
twodimensional
42.2
Gy-Eq.
distributions of neutron beam revealed that thepeak of the beam was a little shifted from thetumor site(Figure 5). For calibration of thebeam peaks to tumor, t is necessary to performa few change the beam direction, and additionof some void to the neighbor site of tumors.

4. Conclusion
Colon26 tumor growth was suppressed in thegroups of BNCT and BNCT with DC injections
relative to controls.
The growth of colon26
tumors was highly suppressed in mice that received
spleen cells from DC-treated mice, suggesting thatanti-tumor immunity was induced by DC
treatment.
Direct DC immunotherapy canenhance the anti-cancer effect of BNCT and havepromising clinical application in near future.

㻙㻌 㻟㻥㻡㻌㻙

5-4

JAEA-Review 2011-050

We applied the JCDS to dosimetry ofepithermal neutron, direction of neutron beam,and patient’s positioning on BNCT. We also
evaluate the epithermal neutron dose to
decreas the skin side effect. High resolution
whole body dosimetry system, as JCDS will bevery useful to evaluate the thermal neutron
dosimetry and the application of BNCT torecurring or advanced breast cancer.

Acknowledgements
This work was supported in part by aGrant-in-Aid from the Ministry of Education,
Science and Culture, Japan (No. 11691202 andNo. 11557092 to Hironobu Yanagie).
Thethermal neutron irradiation was carried out
using the JAEA (Tokai) JRR4 facility supportedby the Inter-University Program for the Joint
Use of JAEA Facilities.

Figure 4. JCDS simulation for rt breast cancer
patient. Upper : lateral view, Lower : frontalview

5. Publications
Yanagie H, et al., 2008. Feasible Evaluationof
NeutronCaptureTherapyfor
Local
Recurrenced Breast Cancer. Proc. of 13th
International Congress of Neutron Capture
Therapy, pp34-37.
Yanagie H, et al., 2008. Inhibition of Tumor
Growth of Mouse Colon Cancer Cell Line by
Boron Neutron Capture Therapy & Immunotherapy. Proc. of 13th International Congress of
Neutron Capture Therapy, pp358-361.
Yanagie H, et al., 2007. Evaluation ofneutron dosimetry on pancreatic cancer
phantom
model
forapplicationof
intraoperative
boron
neutron-capture
therapy, Biomedicine & Pharmacotherapy,
61(9), 505-514.

Figure 5. Two dimensional distributions ofepithermal neutron beam at JRR4 using JCDS
evaluation.

Yanagie H, et al. 2006. Application ofboron-entrapped stealth lipsomes to inhibitionof growth of Tumour cells in the in vivo boron
neutron-capture therapy model; Biomedicine &Pharmacotherapy, 60 : 43-50.

㻙㻌 㻟㻥㻢㻌㻙

5-4

JAEA-Review 2011-050

Yanagie H, et al. 2006. Selective Enhancementof Boron Accumulation with Boron-Entrapped
Water-in-oil-in-water Emulsion in VX-2 Rabbit
Hepatic Cancer Model for BNCT. Proc. of 12th
International Congress of Neutron Capture
Therapy, pp211-214.
Yanagie H, et al. 2006. Production of
Polyoxoboronate as Novel Boron Compound.
Proc. of 12th International Congress of Neutron
Capture Therapy, pp251-252.
Yanagie H, et al. 2006. Application of
Boron-Entrapped WOW Emulsion as borondelivery carrier for boron neutron capture
therapy on VX-2 rabbit hepatic cancer model.
European
Journalof
SurgicalOncology, Volume 32, Supplement 11(1) pp
S19.
ᩉⴡብት㪃㩷 㪉㪇㪇㪏㪅㩷 ਛᕈሶ᝝ᝒ≮ᴺ䈱৻⥸ᄖ⑼㗔ၞ≸䈻䈱ᔕ↪䈫ዷᦸ㪃㩷 ╙ 1 ࿁᧲ᄢ᡼኿✢ࠕ࡜ࠗࠕࡦ
ࠬࡢ࡯࡚ࠢࠪ࠶ࡊ‫ޔ‬2008 ᐕ 3 ᦬ 11 ᣣ‫᧲ޔ‬੩ᄢቇᱞ↰వ┵⍮ࡎ࡯࡞

5-4

㻙㻌 㻟㻥㻣㻌㻙

JAEA-Review 2011-050

߅ ࠊ ࠅ ߦᧄႎ๔ᦠߪ‫⎇ޔ‬ⓥἹ㧔,44‫ޔ‬,44㧕ࠍ೑↪ߒߚ೑↪⠪ߩදജࠍၮߦ‫⎇ޔ‬ⓥἹߩᚑᨐࠍ
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JAEA-Review 2011-050

⻢  ㄉ  ᧄႎ๔ᦠߩ⊒ೀߦ޽ߚࠅ‫ޔ‬ᄙߊߩ⊝᭽߆ࠄᄙᄢߥߏදജࠍ㗂߈߹ߒߚ‫ޕ‬
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0544▤ℂ⺖㐳 ᧛ጊᵗੑ᳁ߦᷓߊᗵ⻢⥌ߒ߹ߔ‫ޕ‬㻙㻌 㻟㻥㻥㻌㻙This is a blank page.

JAEA-Review 2011-050















ઃ ㍳ 


Appendixes㻙㻌 㻠㻜㻝㻌㻙This is a blank page.



JAEA-Review 2011-050

ઃ㍳

ේ⑼⎇⎇ⓥἹߩ೑↪⸳஻৻ⷩ 㧝㧚㧶㧾㧾㧙㧟 㧝㧕ታ㛎⸳஻


ታ 㛎
  ሹ
 
ታ     㛎     ⵝ     ⟎ 㧝㧳   㜞ಽ⸃⢻☳ᧃਛᕈሶ࿁᛬ⵝ⟎㧔㧴㧾㧼㧰㧕        㧝㧳㧙㧭  ↢૕㜞ಽሶ↪ਛᕈሶන⚿᥏࿁᛬ⵝ⟎㧔㧮㧵㨄㧙Υ㧕㧝㧳㧙㧮↢૕㜞ಽሶ↪ਛᕈሶන⚿᥏࿁᛬ⵝ⟎㧔㧮㧵㨄̆Φ㧕 㧞㧳   ਃゲဳਛᕈሶಽశེ㧔㨀㧭㧿㧙㧝㧕 㧟㧳   ♖ኒਛᕈሶశቇⵝ⟎㧔㧼㧺㧻㧕 㧠㧳   ᳢↪ਃゲဳਛᕈሶಽశེ㧔㧳㧼㨀㧭㧿㧕 㧡㧳   ஍ᭂਛᕈሶᢔੂⵝ⟎㧔㧼㧻㧺㨀㧭㧕 㧢㧳   ᧲ർᄢቇਛᕈሶᢔੂಽశེ㧔㨀㧻㧼㧭㧺㧕 㧣㧾   ᾲਛᕈሶ࡜ࠫࠝࠣ࡜ࡈࠖⵝ⟎㧔㨀㧺㧾㧲㧕㨀㧝㧙㧝  ਛᕈሶ஍ᭂ࿁᛬ⵝ⟎㧔㧴㧽㧾㧕㨀㧝㧙㧞  න⚿᥏ਛᕈሶ࿁᛬ⵝ⟎㧔㧷㧿㧰㧕㨀㧝㧙㧟  ☳ᧃਛᕈሶ࿁᛬ⵝ⟎㧔㧷㧼㧰㧕㨀㧝㧙㧠㧙㧝හ⊒ࠟࡦࡑ✢ಽᨆⵝ⟎㧔㧼㧳㧭㧕㨀㧝㧙㧠㧙㧞ᄙ㊀හ⊒ࠟࡦࡑ✢ಽᨆⵝ⟎㧔㧹㧼㧳㧭㧕㨀㧝㧙㧠㧙㧟㨀㧻㧲ဳਛᕈሶ෻኿₸⸘㧔㨀㧻㧲㧕㨀㧝㧙㧠㧙㧠ਛᕈሶ࡜࠙ࠛ࿁᛬ⵝ⟎㧔㧸㧭㨁㧱㧕㨀㧝㧙㧠㧙㧡ਛᕈሶࡌ࡯࠲፣უၮ␆᷹ቯⵝ⟎㨀㧝㧙㧠㧙㧢ᄙ⋡⊛න⦡ᾲਛᕈሶታ㛎ࡐ࡯࠻㧔㜞ⷺ㧕㧔㧹㨁㧿㧭㧿㧵㧕㨀㧞㧙㧝  ਛᕈሶᔕജ᷹ቯⵝ⟎㧔㧾㧱㧿㧭㧕㨀㧞㧙㧞  ਛᕈሶ㧠ゲ࿁᛬ⵝ⟎㧔㧲㧻㧺㧰㧱㧾㧕㨀㧞㧙㧟㧙㧝ᄙ⋡⊛න⦡ᾲਛᕈሶታ㛎ࡐ࡯࠻㧔ૐⷺ㧕㧔㧹㨁㧿㧭㧿㧴㧵㧕㨀㧞㧙㧟㧙㧞   ਛᕈሶᔕജ᷹ቯⵝ⟎㧔㧾㧱㧿㧭㧕㨀㧞㧙㧠㜞ಽ⸃⢻ਃゲဳਛᕈሶಽశེ㧔㨀㧭㧿㧙㧞㧕       㧯㧝㧙㧝  㜞ࠛࡀ࡞ࠡ࡯ಽ⸃⢻ਃゲဳਛᕈሶಽశེ㧔㧴㧱㧾㧕㧯㧝㧙㧞  ੑᰴర૏⟎᷹ቯዊⷺᢔੂⵝ⟎㧔㧿㧭㧺㧿㧙㨁㧕㧯㧝㧙㧟  ⿥㜞ಽ⸃⢻ᓟᣇᢔੂⵝ⟎㧔㨁㧸㧿㧕㧯㧞㧙㧝  ಄ਛᕈሶਃゲဳਛᕈሶಽశེ㧔㧸㨀㧭㧿㧕㧯㧞㧙㧞  ஍ᭂਛᕈሶ෻኿₸⸘㧔㧿㨁㧵㧾㧱㧺㧕㧯㧞㧙㧟㧙㧝ਛᕈሶࠬࡇࡦࠛࠦ࡯ಽశེ㧔㧺㧿㧱㧕㧯㧞㧙㧟㧙㧞㧙㧝 ᄙ㊀හ⊒ࠟࡦࡑ✢ಽᨆⵝ⟎㧔㧹㧼㧳㧭㧕㧯㧞㧙㧟㧙㧞㧙㧞 හ⊒ࠟࡦࡑ✢ಽᨆⵝ⟎㧔㧼㧳㧭㧕㧯㧞㧙㧟㧙㧟㧙㧝 ಄ਛᕈሶ࡜ࠫࠝࠣ࡜ࡈࠖ㧔㧯㧺㧾㧲㧕㧯㧞㧙㧟㧙㧟㧙㧞 ࡄ࡞ࠬਛᕈሶᯏེ㐿⊒ⵝ⟎㧔㧯㧴㧻㧼㧕㧯㧞㧙㧟㧙㧟㧙㧟 㨀㧻㧲ဳਛᕈሶ෻኿₸⸘㧔㨀㧻㧲㧕㧯㧞㧙㧟㧙㧟㧙㧠 ਛᕈሶ࡜࠙ࠛ࿁᛬ⵝ⟎ 㧸㧭㨁㧱 㧯㧟㧙㧝㧙㧝㜞ಽ⸃⢻ࡄ࡞ࠬ಄ਛᕈሶಽశེ㧔㧭㧳㧺㧱㧿㧕㧯㧟㧙㧝㧙㧞㧙㧝 ਛᕈሶశቇࠪࠬ࠹ࡓ⹏ଔⵝ⟎㧔㧺㧻㧼㧕㧯㧟㧙㧝㧙㧞㧙㧞 ᄙጀ⤑ਛᕈሶᐓᷤ⸘㧛෻኿₸⸘㧔㧹㧵㧺㧱㧕㧯㧟㧙㧞  㓸శဳ஍ᭂਛᕈሶ⿥ዊⷺᢔੂⵝ⟎㧔㧿㧭㧺㧿㧙㧶㧕㻙㻌 㻠㻜㻟㻌㻙

JAEA-Review 2011-050

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国際単位系（SI）
表１．SI 基本単位
SI 基本単位

基本量

名称
記号
長
さメ ートル m
質
量 キログラム kg
時
間
秒
s
電
流ア ンペア A
熱力学温度 ケ ル ビ ン K
物 質 量モル mol
光度 カ ン デ ラ cd

表２．基本単位を用いて表されるSI組立単位の例
SI 基本単位
組立量
名称
記号
面
積 平方メートルm2
体
積 立法メートルm3
速 さ ， 速 度 メートル毎秒m/s
加速度 メートル毎秒毎秒
m/s2
波
数 毎メートルm-1
密 度 ， 質 量 密 度 キログラム毎立方メートル
kg/m3
面
積
密
度 キログラム毎平方メートル
kg/m2
比
体
積 立方メートル毎キログラム
電流
密
度 アンペア毎平方メートル
磁 界 の 強 さ アンペア毎メートル
量 濃 度 (a) ， 濃 度 モル毎立方メートル
質量
濃度 キログラム毎立法メートル
輝
度 カンデラ毎平方メートル屈折率 (b) （数字の） １
比 透 磁 率 (b) （数字の） １

乗数
24

10
1021
1018
1015
1012
109
106
103

3

m /kg
A/m2
A/m
mol/m3
kg/m3
cd/m2
1
1

102
101

表５．SI 接頭語
記号 乗数
接頭語
Ｙ
シ
10-1 デ

ゼ
タ
エ ク サ

Ｚ
Ｅ

10-2

ペ
テ

タ
ラ

Ｐ
Ｔ

ギ
メ

ガ
ガ

Ｇ
Ｍ

マイクロ
ノ
10-9 ナコ
10-12 ピ
10-15 フェムト

キ
ロ
ヘ ク ト
デ
カ

ｋ
ｈ
da

10-3
10-6

記号

セ ン チ
ミ
リ

ト
10-18 ア
10-21 ゼ プ ト
10-24 ヨ ク ト

d

c
m
µ
n
p
f
a
z
y

表６．SIに属さないが、SIと併用される単位
名称
記号
SI 単位による値
分
min 1 min=60s
時
h 1h =60 min=3600 s（a）量濃度（amount concentration）は臨床化学の分野では物質濃度（substance concentration）ともよばれる。
（b）これらは無次元量あるいは次元１をもつ量であるが、そのことを表す単位記号である数字の１は通常は表記しない。

d
°
’

日
度
分

表３．固有の名称と記号で表されるSI組立単位
SI 組立単位
組立量
他のSI単位による SI基本単位による
名称
記号
表し方
表し方
（ｂ）
平
面
角 ラジアン(ｂ)
rad
m/m
1
（ｂ）
(ｂ)
(c)
2/ 2
立
体
角 ステラジアン
sr
1
m m
周
波
数 ヘルツ（ｄ）
Hz
s-1
力
ニュートン
N
m kg s-2
圧力
応
力 パスカル,Pa
m-1 kg s-2
N/m2
エ ネ ル ギ ー , 仕 事 , 熱 量 ジュールJNm
m2 kg s-2
仕 事 率 ， 工 率 ， 放 射 束 ワット
WJ/s
m2 kg s-3
電
荷
電気量 クーロン,
CsA
電 位 差 （ 電 圧 ） , 起 電 力 ボルト
VW/A
m2 kg s-3 A-1
静電
容量 ファラドF
C/V
m-2 kg-1 s4 A2
電
気
抵
抗 オーム
Ω
V/A
m2 kg s-3 A-2
コ ン ダ ク タ ン ス ジーメンス
S
A/V
m-2 kg-1 s3 A2
磁
束 ウエーバWb
Vs
m2 kg s-2 A-1
磁
束
密
度 テスラ
T
kg s-2 A-1
Wb/m2
イ ン ダ ク タ ン ス ヘンリーH
Wb/A
m2 kg s-2 A-2
セ ル シ ウ ス 温 度 セルシウス度(ｅ)℃K
光
束 ルーメンlm
cd
cd sr(c)照度 ルクスlx
m-2 cdlm/m2
Bqs-1
放 射 性 核 種 の 放 射 能 （ ｆ ） ベクレル（ｄ）
吸収線量, 比エネルギー分与,
グレイ
Gy
J/kg
m2 s-2カーマ
線量当量, 周辺線量当量, 方向
Sv
J/kg
m2 s-2シーベルト（ｇ）
性線量当量, 個人線量当量酸素
活性 カタールkat
s-1 mol

1 d=24 h=86 400 s
1°=(π/180) rad1’=(1/60)°=(π/10800) rad”1”=(1/60)’=(π/648000) radha 1ha=1hm2=104m2
L，l 1L=11=1dm3=103cm3=10-3m3t
1t=103 kg

秒
ヘクタール
リットル
トン

表７．SIに属さないが、SIと併用される単位で、SI単位で表される数値が実験的に得られるもの
名称
記号
SI 単位で表される数値
電 子 ボ ル ト
ダ ル ト ン
統一原子質量単位

eV
Da
u

天

ua

文

単

位

1eV=1.602 176 53(14)×10-19J

1Da=1.660 538 86(28)×10-27kg
1u=1 Da1ua=1.495 978 706 91(6)×1011m

表８．SIに属さないが、SIと併用されるその他の単位
名称
記号
SI 単位で表される数値
バー
ル bar １bar=0.1MPa=100kPa=105Pa
水銀柱ミリメートル mmHg 1mmHg=133.322Pa(a)SI接頭語は固有の名称と記号を持つ組立単位と組み合わせても使用できる。しかし接頭語を付した単位はもはや
コヒーレントではない。
(b)ラジアンとステラジアンは数字の１に対する単位の特別な名称で、量についての情報をつたえるために使われる。
実際には、使用する時には記号rad及びsrが用いられるが、習慣として組立単位としての記号である数字の１は明示されない。
(c)測光学ではステラジアンという名称と記号srを単位の表し方の中に、そのまま維持している。
(d)ヘルツは周期現象についてのみ、ベクレルは放射性核種の統計的過程についてのみ使用される。
(e)セルシウス度はケルビンの特別な名称で、セルシウス温度を表すために使用される。セルシウス度とケルビンの単位の大きさは同一である。したがって、温度差や温度間隔を表す数値はどちらの単位で表しても同じである。
(f)放射性核種の放射能（activity referred to a radionuclide）は、しばしば誤った用語で”radioactivity”と記される。
(g)単位シーベルト（PV,2002,70,205）についてはCIPM勧告2（CI-2002）を参照。

表４．単位の中に固有の名称と記号を含むSI組立単位の例
SI 組立単位
組立量
SI 基本単位による
名称
記号
表し方
-1
粘
度 パスカル秒
Pa s
m kg s-1
力 の モ ー メ ン ト ニュートンメートル
Nm
m2 kg s-2
表面
張力 ニュートン毎メートル
N/m
kg s-2角
速度 ラジアン毎秒
rad/s
m m-1 s-1=s-1
角
加速度 ラジアン毎秒毎秒
rad/s2
m m-1 s-2=s-2
熱 流 密 度 , 放 射 照 度 ワット毎平方メートル
W/m2
kg s-3
熱 容 量 , エ ン ト ロ ピ ー ジュール毎ケルビン
J/K
m2 kg s-2 K-1
比 熱 容 量 ， 比 エ ン ト ロ ピ ー ジュール毎キログラム毎ケルビン J/(kg K)
m2 s-2 K-1
比 エ ネ ルギ ー ジュール毎キログラム
J/kg
m2 s-2
熱伝
導率 ワット毎メートル毎ケルビン W/(m K) m kg s-3 K-1
体 積 エ ネ ル ギ ー ジュール毎立方メートル J/m3
m-1 kg s-2
電界の強さ ボルト毎メートル
V/m
m kg s-3 A-1
電荷密
度 クーロン毎立方メートル C/m3
m-3 sA
表面
電
荷 クーロン毎平方メートル C/m2
m-2 sA
電 束 密 度 ， 電 気 変 位 クーロン毎平方メートル C/m2
m-2 sA誘
電率 ファラド毎メートル
F/m
m-3 kg-1 s4 A2
透磁率 ヘンリー毎メートル
H/m
m kg s-2 A-2
モ ル エ ネ ル ギ ー ジュール毎モル
J/mol
m2 kg s-2 mol-1
モルエントロピー, モル熱容量 ジュール毎モル毎ケルビン J/(mol K) m2 kg s-2 K-1 mol-1
照 射 線 量 （ Ｘ 線 及 び γ 線 ） クーロン毎キログラム
C/kg
kg-1 sA
吸収線
量率 グレイ毎秒
Gy/s
m2 s-3放射
強度 ワット毎ステラジアン
W/srm4 m-2 kg s-3=m2 kg s-3
放射輝
度 ワット毎平方メートル毎ステラジアン W/(m2 sr) m2 m-2 kg s-3=kg s-3
酵 素 活 性濃 度 カタール毎立方メートル kat/m3
m-3 s-1 mol

接頭語
ヨ
タ

オングストローム
海
里
バ
ー
ン

Å
Ｍ

１Å=0.1nm=100pm=10-10m
１M=1852m

b

ノ
ネ
ベ

ト
パ
ル

kn
Np
Ｂ

１b=100fm2=(10-12cm)2=10-28m2
１kn=(1852/3600)m/s

ル

dB

ッ
ー

デ

ジ

ベ

SI単位との数値的な関係は、対数量の定義に依存。

エ

表９．固有の名称をもつCGS組立単位
名称
記号
SI 単位で表される数値
ル
グ erg 1 erg=10-7 J

ダ
ポ

イ
ア

ス
ス

ト ー ク
チ
ル

フ
ガ

ォ

ン dyn 1 dyn=10-5N
ズ P 1 P=1 dyn s cm-2=0.1Pa s
ス St 1 St =1cm2 s-1=10-4m2 s-1
ブ sb 1 sb =1cd cm-2=104cd m-2
ト ph 1 ph=1cd sr cm-2 104lx
ル Gal 1 Gal =1cm s-2=10-2ms-2

マ ク ス ウ ｪ ルガ
ウス
エルステッド（ ｃ）

Mx
G
Oe

1 Mx = 1G cm2=10-8Wb

1 G =1Mx cm-2 =10-4T
1 Oe (103/4π)A m-1（c）３元系のCGS単位系とSIでは直接比較できないため、等号「は対応関係を示すものである。

キ
レ
ラ

名称
ュ
リ
ン

レ
ガ

ト

表10．SIに属さないその他の単位の例
記号
SI 単位で表される数値
ー Ci 1 Ci=3.7×1010Bq

ゲ

ン

ン R
ド rad
ム rem
マ γ

1 R = 2.58×10-4C/kg

1 rad=1cGy=10-2Gy
1 rem=1 cSv=10-2Sv
1γ=1 nT=10-9T

1フェルミ=1 fm=10-15m

フェルミ
メートル系カラット

1メートル系カラット = 200 mg = 2×10-4kg

気

ル Torr 1 Torr = (101 325/760) Pa
圧 atm 1 atm = 101 325 Pa

ロ

リ

ー

cal

ク

ロ

ン

µ

ト
標

準

カ
ミ

大

」

1cal=4.1858J（｢15℃｣カロリー），4.1868J（｢IT｣カロリー）4.184J（｢熱化学｣カロリー）

1 µ =1µm=10-6m（第8版，2006年改訂）

この印刷物は再生紙を使用しています