本レポートは独立行政法人日本原子力研究開発機構が不定期に発行する成果報告書です。
本レポートの入手並びに著作権利用に関するお問い合わせは、下記あてにお問い合わせ下さい。
なお、本レポートの全文は日本原子力研究開発機構ホームページ（http://www.jaea.go.jp）
より発信されています。
独立行政法人日本原子力研究開発機構〒319-1195

研究技術情報部

研究技術情報課

茨城県那珂郡東海村白方白根 2 番地 4

電話 029-282-6387, Fax 029-282-5920, E-mail:ird-support@jaea.go.jp
This report is issued irregularly by Japan Atomic Energy Agency.
Inquiries about availability and/or copyright of this report should be addressed toIntellectual Resources Section, Intellectual Resources Department,
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Tel +81-29-282-6387, Fax +81-29-282-5920, E-mail:ird-support@jaea.go.jp© Japan Atomic Energy Agency, 2014

JAEA-Review 2013-039

研究炉（JRR-3 及び JRR-4）利用における研究成果集（平成２０年度）

日本原子力研究開発機構 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（編）研究炉利用課（2013 年 9 月 24 日受理）

JRR-3 は、中性子散乱、即発ガンマ線分析、中性子ラジオグラフィなどの実験利用、及び、放射化分析、原子炉燃料材料、ラジオアイソトープ製造、フィッショントラック
年代測定の照射利用など、様々な目的に利用されている。
JRR-4 については、医療照射（Boron Neutron Capture Therapy：BNCT）、即発ガンマ
線分析、放射線測定器の感度試験、原子炉研修運転実習等の実験利用、及び、放射化分
析、ラジオアイソトープ製造、フィッショントラック年代測定のための照射利用など、様々な目的に利用されている。
平成 20 年度、研究炉 JRR-3 は 7 サイクルの運転（1 サイクル：26 日連続運転）の施
設共用運転を行なった。研究炉 JRR-4 は反射体要素の吊り手溶接部に割れが発見され、取り替え用反射体要素の製作及び交換が必要となったため、運転は行われなかった。
本報告書は、平成２０年度に実施した施設利用成果の提出を研究炉の利用者（原子力機構外を含む）から受け、中性子散乱 11 分野（構造、磁性、超伝導など）、中性子ラジオグラフィ、放射化分析、その他、の分野別についてその研究成果を取りまとめたものである。

原子力科学研究所：〒319-1195

茨城県那珂郡東海村白方白根 2-4i

JAEA-Review 2013-039

Activity Report on the Utilization of Research Reactors (JRR-3 and JRR-4)(Japanese Fiscal Year, 2008)(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 September 24, 2013)
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 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 tracksetc.
In the fiscal year 2008, the research reactor JRR-3 was operated for 7 cycles (cycle operation :26days/cycle) for utilization sharing of facility.
The research reactor JRR-4 was not operated in 2008. Because a crack was found on the weld of
the aluminum cladding of a graphite reflector element. JRR-4 has remained shutdown until thereflector elements were replaced.
The volume contains 250activity reports, which are categorized into the fields of neutron
scattering (11 subcategories), neutron radiography, neutron activation 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, Irradiationii

JAEA-Review 2013-039

目

はじめに

次

·························································

1

研究成果一覧 ······················································

3

1. 中性子散乱 ····················································

211) 構造・励磁 ················································· 212) 磁性 ·····················································

713) 強相関電子系 ··············································· 139
4) 非晶質･液体 ················································ 1715) 高分子 ····················································· 185
6) 生

物 ····················································· 237

7) 基礎物理学･中性子光学 ······································· 2518) 装

置 ····················································· 257

9) 超伝導現象 ················································· 279
10) 残留応力 ··················································· 283
11) その他 ····················································· 2932.

中性子ラジオグラフィ ·········································· 299

3.

放射化分析 ··················································· 309

4.

その他 ······················································· 411

おわりに························································· 415

謝辞····························································· 416

付録····························································· 417

iii

JAEA-Review 2013-039

Contents··························································

1

Research Reports ··················································

3

1. Neutron Scattering ··············································

211) Structure･Excitation ···········································

212) Magnetism ··················································

71

Preface3) Strongly Correlated Electron Systems···························· 139

4) Amorphous・Liquid ··········································· 171
5) Polymer···················································· 185

6) Biology···················································· 237

7) Fundamental Physics・Neutron Optics ···························· 251
8) Instrument·················································· 257

9) Superconductivity10) Residual Stress11) Others············································ 279·············································· 283····················································· 293

2. Neutron Radiography ············································ 299
3. Neutron Activation Analyses····································· 309

4. Others ························································ 411
Conclusion························································ 415

Acknowledgments ··················································· 416
Appendixes ························································ 417

iv

JAEA-Review 2013-039

は じ め に

平成２０年度には、ＪＲＲ－３において７サイクルの共同利用運転が行われ、これに伴いさまざまな利用が行われた。ＪＲＲ－４については取り替え用反射体要素の製作及び交換が必要となったため、運転は行われなかった。
本報告書は、利用者（原子力機構外利用者を含む）から当該利用の成果の提出を受け、取りまとめたものである。
提出して頂いた成果の件数は、中性子散乱２２３件、中性子ラジオグラフィ５件、放射化分析２１件、その他１件で合計２５０件であった。なお、本報告書の一部は、貴重な研究成果を公開する機会を広げるため、下記報告書の中から転載させて頂いたものである。
最後に、原稿を提出して頂いた利用者の皆様のご協力に感謝するとともに、今後も研究炉が有効に利用され、種々の研究がさらに進展されることを期待します。
研究炉利用課長
笹島 文雄

1)標題 ：ACTIVITY REPORT ON NEUTRON SCATTERINGRESEARCH issued by ISSP-NSL,University of Tokyo,Vol.16（東京大学物性研究所発行）

編者 ：東京大学物性研究所

発 行 年 ：２００９年
2)標編

題 ：原子力機構施設利用総合共同研究成果報告集（平成２０年度）
者 ：東京大学大学院工学系研究科原子力専攻共同利用管理本部

発 行 年 ：２００９年- 1-This is a blank page.

JAEA-Review 2013-039

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JAEA-Review 2013-039

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1-1-101-1-111-1-121-1-131-1-141-1-151-1-16
1-1-171-1-181-1-19
1-1-201-1-21
1-1-22「 Title 」
Neutron Scattering - Structure ・ Excitation Phonon Dispersion Relations of LaAlO3-SrTiO3
H. Yamauchi, T. Shimada, K. Ichikawa, J. Breeze, N. McN Alford
Crystal Structure and Nuclear Density Distribution of LiCo1/3Ni1/3Mn1/3O2
Analyzed by Applying Rietveld/Maximum Entropy Method
N. Igawa, T. Taguchi, H. Fukazawa, H. Yamauchi, W. Utsumi
Neutron Powder Diffraction Study of Water-Dissolved Ba2In2O5
T. Nagasaki, S. Shiotani, M. Yoshino, K. Iwasaki, N. Igawa, H. Fukazawa, H. Yamauchi, W. Utsumi
Structure of Ice XI and a New Form, Ice XV
H. Fukazawa
Correlation Effects among Thermal Displacements of Atoms in KBr
T. Sakuma, Xianglian, N. Shimizu, J. Yokokawa, H. Takahashi, N. Igawa
Effect of Consolidation Condition on Nano-size Oxide Particle Dispersion in 9Cr-ODS Steel
S. Ohtsuka, J. Suzuki, T. Kaito, M. Inoue, S. Kim, S. Obara, T. Asayama
Nano-structure analysis of high Cr steel for long life FBR structural material
S. Obara, J. Suzuki, T. Wakai, S. Ohtsuka, M. Inoue, T. Asayama
Development of High Pressure Device for Neutron Powder Diffraction－ Feasibility Test using Lanthanum Hydride －W. Utsumi, T. Hattori, A. Machida, N. Igawa
Study of Mesoscale Spatial Distribution of Electron Spins in High Crystallinity
Polyethylene Doped with TEMPO Using Time-Resolved Dynamic Nuclear
Polarization and Small-Angle Neutron Scattering Methods
T. Kumada, Y. Noda, S. Koizumi, T. HashimotoHigh Temperature Neutron Diffraction Study of (La0.5Sr0.5)CoO3-d Perovskite
K. Nomura, H. Kageyama, K. Kakinuma, T. Maekawa, S. Nakamura, H. Miyazaki, H. Imabayashi,
T. Ito, M. Yashima
Structural Disorder and Diffusional Pathway of Oxide Ions in a Doped
Pr2NiO4-Based Mixed Conductor
M. Yashima, M. Enoki, T. Wakita, R. Ali, Y. Matsushita, F. Izumi, T. Ishihara
Neutron diffraction study of Yb compounds
M. Kurisu, H. Murakami, G. Nakamoto, T. Tsutaoka, Y. Andoh
Measurement of over dumped phonon on protonic conductor K3H(SeO4)2
F. Shikanai, S. Itoh, K. Tomiyasu, N. Aso, T. J. Sato, S. Ikeda, T. Kamiyama
Phonon dispersion of off-stoichiometric Ni2MnGa sigle crystal
K. Inoue, Y. Yamaguchi, H. Hiraka
Structure and Magnetism of Infinite Layer Iron Oxide with a Square-Planar Coordination
C. Tassel, Y. Tsujimoto, H. Kageyama, K. Yoshimura, M. Takano, M. Nishi, K. Ohoyama
Observation of the spin gap in a two-dimensional quantum spin system (CuCl)Ca2Nb3O10
Y. Tsujimoto, H. Kageyama, K. Yoshimura, Y. Ajiro, M. Nishi
Behavior of Thermal Parameters and the Phase Transition in DKDP
H. Mashiyama, T. Miyoshi, T. Asahi, H. Kimura, Y. Noda
Correlation between crystal defects and the diffuse scattering in relaxor
ferroelectric (Na0.5Bi0.5)TiO3
M. Matsuura, K. Hirota, Y. Noguchi, M. Miyayama
Temperature dependence of waterfall feature of phonons in (Na0.5Bi0.5)TiO3
M. Matsuura, K. Hirota, Y. Noguchi, M. Miyayama
Study of slow lattice dynamics in relaxor PMN-30%PT by neutron spin echo technique
M. Matsuura, H. Endo, K. Hirota
Pseudospin-phonon coupling in Relaxor Ferroelectrics PMN-x%PT
M. Matsuura, K. Hirota
Crystal structure analysis in pressure-induced commensurate magnetic phase ofmultiferroic HoMn2O5
H. Kimura, Y. Sakamoto, T. Yamazaki, Y. Noda, N. Aso, T. Fujiwara, K. Matsubayashi,
Y. Uwatoko

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1-1-23 Hypothetical Phase Transitions and soft modes in A2BX4-type Dielectrics
H. Shigematsu, K. Nomura
1-1-24 Crystal and magnetic structure of multiferroic material BiFeO3-BaTiO3
R. Kiyanagi, T. Yamazaki, Y. Sakamoto, H. Kimura, Y. Noda, K. Ohyama
1-1-25 Phase transition in a lead-based inorganic-organic perovskites C5H10NH2PbI3
M. Takahashi, M. Nakatsuma, K. Kataoka, T. Kawasaki, K. Ohshima, Y. Noda
1-1-26 Magnetic Fluctuations in a Ternary Alloy CuFePt6
M. Takahashi, T. Shishido, K. Ohshima, M. Matsuura
1-1-27 Kinetics of crystalline-noncrystalline phase transition of sucrose crystal
M. Takahashi, K. Kawasaki, K. Ohshima
1-1-28 Crystal structure of Pb-free silver niobate perovskite
M. Yashima, T. Wakita, T. Komatsu, Y. Phat, H. Taniguchi, T. Taniyama, M. Itoh
1-1-29 Structure Analysis of Oxide Ions in a Doped Pr2NiO4-based Mixed Conductor
H. Yamada, M. Yashima, T. Takizawa, S. Yamamoto, T. Ishihara
1-1-30 Structure analysis of automotive exhaust catalysts, Ce2Zr2O7.32 by neutron
powder diffraction measurement
T. Takizawa, M. Yashima, T. Wakita
1-1-31 Lattice dynamics of cubic NaNbO3
I. Tomeno, Y. Tsunoda, K. Oka, M. Matsuura, M.Nishi
1-1-32 Phonons in tetragonal BiVO4
I. Tomeno, N. Sato, K. Oka
1-1-33 Inelastic neutron scattering in the impurity-induced ferroelectric phase of CuFe1 yGayO2
1-1-34
1-1-35
1-1-36
1-1-37

1-1-38
1-1-39

1-1-401-1-41

1-1-42

1-1-43
1-1-441-1-45

N. Terada, T. Nakajima, S. Mitsuda
Crystal structure analyses of layered thermoelectric manganites
Y. Miyazaki, F. Kawashima, K. Hayashi, T. Kajitani
Low-Energy Phonon Anomaly of CeRu4Sb12
K. Iwasa, R. Igarashi, L. Hao, Y. Murakami
Neutron Diffraction Study on SnO2-MOx (M = Ce, Sb) System
K. Nomura, H. Kageyama, T. Maekawa, C. Minagoshi, H. Miyazaki, Y. Kawabata
Observation of Hydrogen Tunneling in Pd nanoparticles by Low-temperature
Neutron Scattering Measurement
M. Yamauchi, H. Kitagawa, O. Yamamuro
Structural, magnetic and thermoelectric properties of half-Heusler compounds
G. Nakamoto, H. Murakami, M. Kurisu, A. Tanaka, T. Tsutaoka, Y. Andoh
Dependence of crystal structure and thermodynamic stability on different
synthetic method and Li content for Lix(Ni,M)O2 (M=Mn,Co) as a cathodeactive material for Li ion battery
Y. Idemoto, N. Kitamura, T. Hasegawa
Crystal structure and ionic conduction path of Ln2Ni1-xCuxO4+d for solid oxide fuel cells
Y. Idemoto, N. Kitamura
Structural Analysis of Interface between DLC films Having Various Wettabilities
and Lubricants Using Neutron Reflectometry
T. Hirayama, T. Torii, T. Kashihara, T. Matsuoka, K. Inoue, M. HinoHigh Temperature Neutron Diffraction Study of (La0.6Sr0.4)(Co0.8Fe0.2)O3-d Perovskite
K. Nomura, K. Kakinuma, T. Kojima, N. Takeichi, H. Kageyama, T. Maekawa, C. Minagoshi,
H. Miyazaki, Y. Kawabata
Phonons in FCC-Fe precipitates in Cu
K. Horiguchi, Y. Tsunoda
Crystal Structure Analysis of a Supramolecular Ferroelectric 55DMBP-H2ia at
Low-temperature Phase
R. Kumai, D. Okuyama, S. Horiuchi, T. Arima, R. Kiyanagi, Y. Noda, Y. Tokura
Crystal Structure of Lithium Battery Electrode Materials with Tunnel Structure
N. Kijima, J. Akimoto, K. Kataoka

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1-2-7
1-2-8
1-2-9
1-2-101-2-11
1-2-121-2-131-2-141-2-151-2-16

1-2-171-2-181-2-19
1-2-20「 Title 」
Neutron Scattering - Magnetism Magnetic Bragg Peaks of Quasi-One-Dimensional Antiferromagnets
Cu6Ge6O18-xD2O (x = 0, 6)
M. Hase, N. Terada, H. S. Suzuki, H. Kitazawa, K. Ozawa, K. Kaneko, N. Metoki, M. Matsuda,
K. Kakurai
Spherical Neutron Polarimetry Analysis in the Ferroelectric Phase of theMagnetoelectric Multiferroic CuFe1−yGayO2
N. Terada, T. Nakajima, S. Mitsuda, M. Matsuda, K. Kakurai, H. Kitazawa
Magnetic and Structural Phase Transitions of RbFeBr3
Y. Nishiwaki, K. Kakurai, T. Kato
Crystal Structure Analysis and Magnetic Properties of Multiferroic System
Ni3(1−x)Cu3xV2O8
T. Kai, Y. Yasui, M. Sato, H. Fukazawa, N. Igawa, K. Kakurai
Studies of Multiferroic System of LiCu2O2 -Magnetic Structures of Two Ordered
Phases with Incommensurate ModulationsK. Sato, Y. Yasui, T. Moyoshi, Y. Kobayashi, M. Sato, K. Kakurai
Crystal-Field Study of Clathrate Rare-Earth Compounds Ce3Pd20(Si1−xGex)6
with Multi-Polar Ordering
H. Kitazawa, N. Terada, Y. Tsuchiya, Y. Kawamura, A. Kikkawa, A. Dönni, O. Sakai,
M. Matsuda, K. Kakurai, Y. Nemoto, T. Goto
Enhancement of the Two-Dimensional Spin Correlations in Ag doped CuCrO2
R. Kajimoto, M. Matsuda, T. Kishimoto, K. Uto, T. Hokazono, T. Okuda
Dynamical Character of the Two-Dimensional Spin Correlations in Ag doped CuCrO2
R. Kajimoto, M. Matsuda, T. Kishimoto, K. Uto, T. Hokazono, T. Okuda
Spin Correlations in a Frustrated Spinel Antiferromagnet LiCrMnO4
M. Matsuda, Z. Honda, H. A. Katori, H. Takagi, H. Ueda, Y. Ueda, H. Mitamura, K. Kindo
Magnetic Field-Induced Transitions in the Spinel GeCo2O4
M. Matsuda, T. Hoshi, H. A. Katori, M. Kosaka, H. Takagi
High-Pressure Neutron Diffraction Study of Magnetic Properties in DyB2C2
H. Yamauchi, T. Osakabe
Nematic-to-Smectic Transition of Magnetic Texture in Conical State
M. Takeda, Y. Endoh, K. Kakurai, Y. Onose, J. Suzuki, Y. Tokura
Anisotropic Spin Freezing in Lightly-Doped La2−xSrxCuO4
M. Matsuda, M. Fujita, M. Takeda, K. Kakurai, K. Yamada
Magnetic Structural Analysis of Magnetic Multilayers for Read Sensor Heads
by Polarized Neutron Reflectometry
M. Takeda, D. Yamazaki, T. Hirano
Acquirement of a Guiding Principle Towards the Dy-free or Dy-lessHigh Performance Nd-Fe-B Sintered Magnets
by Investigation of the Origin of the Coercivity with Interfacial Structural Analysis
M. Takeda, J. Suzuki, D. Yamaguchi, T. Akiya, H. Kato, Y. Une, M. Sagawa
Polarized Neutron Diffraction Study of Magnetic Chirality in Multiferroic
Compound TmMn2O5
S. Wakimoto, H. Kimura, M. Fukunaga, M. Takeda, K. Kakurai, Y. Noda
A Small-Angle Polarized Neutron Scattering Experiment of Spherical
Fe16N2 Nano-Particles for High Density Magnetic Recording Tape
H. Hagiya, T. Oku, H. Kira, T. Shinohara, J. Suzuki, Y. Tamai, M. Takeda, K. Kakurai,
Y. Sasaki, M. Kishimoto, M. Yokoyama, Y. Nishihara
Magnetic Structure in the Shastry-Sutherland Lattice TmB 4
F. Iga, A. Shigekawa, S. Michimura, T. Takabatake, S. Yoshii, T. Yamamoto, M. Hagiwara,
K. Kindo, K. Ohoyama
Successive metamagnetic behavior in an easy-plane type antiferromagnet ErNi2Ge2
Y. Tabata, M. Okue, H. Nakamura, N. Matsuura
Anisotropic magnetic diffuse scattering in an easy-plane type antiferromagnet ErNi2Ge2
Y. Tabata, H. Taguchi, K. Matsuda, H. Nakamura

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1-2-21 Magnetic structure of RCoSn (R=Tb, Ho and Er)
M. Kurisu, G. Nakamoto, T. Tsutaoka, Y. Andoh
1-2-22 Relationship between Magnetic Structure and Ferroelectricity of LiCu2O2
Y. Yasui, K. Sato, Y. Kobayashi, T. Moyoshi, M. Sato, K. Kakurai
1-2-23 Magnetic Properties of Honeycomb System Na2Co2TeO6
Y. Yasui, Y. Miura, T. Moyoshi, M. Sato, K. Kakurai
1-2-24 Magnetic structure of multiferroic DyMnO3 studied by polarized neutron diffraction
D. Okuyama, H. Murakawa, K. Iwasa, H. Sagayama, Y. Kaneko, Y. Taguchi, T. Arima, Y. Tokura
1-2-25 Neutron Diffraction Studies on Dy7Rh3Dx
T. Tsutaoka, A. Tanaka, G. Nakamoto, M. Kurisu, Y. Andoh, R. Sato, S. M. Filipek
1-2-26 Quantum Phase Transition in the Solid Solution
A. Kitada, Y. Tsujimoto, H. Kageyama, K. Yoshimura, M. Nishi
1-2-27 Electric polarization flop induced by magnetic phase transition in multiferroic YbMn2O5
H. Kimura, Y. Sakamoto, M. Fukunaga, Y. Noda, H. Hiraka
1-2-28 Relationship between Spin Helicity and Electric Polarization in Multiferroic Material
CuCrO2
M. Soda, K. Kimura, T. Kimura, M. Matsuura, K. Hirota
1-2-29 Competition between Relaxor-like behavior and Magnetic Ordering in(1-x)BiFeO3-xBaTiO3
M. Soda, K. Hirota
1-2-30 Magnetic structure analysis of Crednerite CuMnO2
N. Terada
1-2-31 Long-time variation of magnetic structure in a multistep metamagnet CeIr3Si2
K. Motoya, Y. Muro, T. Takabatake
1-2-32 Inelastic neutron scattering study in O2 adsorbed deuterated CPL-1
T. Masuda, S. Hondo, M. Matsuuda
1-2-33 Chiral Helimagnetic Order in T1/3NbS2 (T=Cr, Mn)
Y. Kousaka, Y. Nakao, H. Furukawa, J. Akimitsu
1-2-34 Neutron powder diffraction of Tb1-xGdxB2C2(x=0.15,0.2)
E. Matsuoka, Y. Sasaki, K. Ohoyama, H. Onodera
1-2-35 Elastic diffuse scattering of neutrons in Fe3Pt Invar alloys
M. Takasaka, Y. Tsunoda
1-2-36 Refinement of magnetic structure in the ferroelectric phase of Cu(Fe,Ga)O2
T. Nakajima, S. Mitsuda, K. Yoshitomi, H. Kimura, Y. Noda
1-2-37 Magnetic Structure in Ba2Mg2Fe12O22
H. Sagayama, K. Taniguchi, T. Arima, Y. Nishikawa, S. Yano, J. Akimitsu, H. Kimura, Y. Noda
1-2-38 Effective random-fied domain-state in Ga-substituted CuFeO2
T. Nakajima, S. Mitsuda, M. Yamano, H. Yamazaki, K. Kuribara
1-2-39 Competing Interactions in Two Dimensional Square Lattice CuSb2-xTaxO6
M. Nishi, M. Kato, K. Hirota
1-2-40 Spin-driven dielectric relaxation in a paraelectric phase of magneto-electric
multiferroic CuFeO2
S. Mitsuda, M. Yamano, K. Kuribara, T. Nakajima, K. Masuda, K. Yoshitomi
1-2-41 Inelastic Neutron Scattering Study on Triangular Lattice Antiferromagnet CuCrO2
T. Nozaki, K. Hayashi, T. Kajitani
1-2-42 Observation of magnetic fluctuation in Ni2(OD)3Cl by neutron scattering
Y. Oohara, M. Hagihala, X.G. Zheng
1-2-43 Study of spin gap in two-dimensional frustrated triangular lattice: YbAl3C3
M. Kosaka, T. Kobiyama, A. Yamada, K. Ohoyama, N. Aso
1-2-44 Spin Waves in MnPS. Yano, M. Nishi, M. Matsuura, K. Hirota, J. Akimitsu
1-2-45 Spin Waves in MnPS. Yano, K. Iwasa, J. Akimitsu
1-2-46 Research for magnetic reflections on HoRh2Si2
T. Shigeoka, A. Tanaka, G. Nakamoto
1-2-47 Neutron scattering study on the magnetic moleculars
K. Iida, H. Ishikawa, T. Yamamse, T. J Sato

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1-2-48 Crystal Field Softeing and Magnetic Phase Transition in HoB4
T. Matsumura, D. Okuyama
1-2-49 Phase Transitions of Non-Kramers Pr Ions in a Trigonal Symmetry in Pr4Ni3Pb4
T. Onimaru, A. Ishida, K. Shigetoh, Y. F. Inoue, M. Nishi, T. J. Sato, Y. Oohara, T. Takabatake
1-2-50 Giant Uniaxial Anisotropy in the Magnetic and Transport Properties of CePd5Al2
T. Onimaru, Y. F. Inoue, K. Ohoyama, T. Takabatake
1-2-51 Magnetic structure of Nd0.33Sr1.66MnO4
Y. Oohara, M. Kubota, H. Kuwahara
1-2-52 Magnetic excitations in YbV4O8
Y. Oohara, M. Kubota, Y. Kanke
1-2-53 Multiple temperature and field induced phase transitions in new geometricfrustration material Co2(OH)3Br
M. Hagihala, X. G. Zheng, T. J Sato
1-2-54 Neutron powder diffraction of TbPd3S4 in magnetic fields
E. Matsuoka, Y. Sasaki, T. Matsumura, K. Ohoyama, H. Onodera
1-2-55 Inelastic neutron scattering study on 1/1 approximant Ag-In-Tb
S. Ibuka, K. Matan, T. J. Sato
1-2-56 Neutron scattering study on magnetic quasicrystal Zn-Mg-(Y,Gd)
S. Ibuka, K. Iida, T. J. Sato
1-2-57 Magnetic structures in magnetic fields of TmB4 with the Shastry-Sutherland latticeF. Iga, S. Michimura, T. Matsumura, T. Takabatake, K. Ohoyama
1-2-58 Magnetic State in the Tm-based Reentrant Superconductor Investigated by the
Powder Neutron Scattering
N. Kase, Y. Tomiyasu, T. Muranaka, J. Akimitsu
1-2-59 Neutron diffraction experiment under high pressure in YbMn2Ge2
T. Fujiwara, N. Aso, M. Nishi, Y. Uwatoko
1-2-60 Magnetic excitation in Co4B6O13
T. Masuda, S. Hondo, M. Matsuura
1-2-61 Degree of frustration in geometrically frustrated magnets (Co1-xZnx)Cr2O4
K. Tomiyasu, T. Yokobori, K. Horigane, J. Akimitsu, K. Yamada

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1-3-2
1-3-3
1-3-4
1-3-5
1-3-6
1-3-7
1-3-8

1-3-9
1-3-101-3-11
1-3-12
1-3-131-3-141-3-151-3-16
1-3-171-3-181-3-19
1-3-201-3-21
1-3-22
1-3-231-3-241-3-25「 Title 」
Neutron Scattering - Strongly Correlated Electron SystemsCompetition of different antiferromagnetic correlations in a heavy fermion
Ce(Ru1-xRhx)2(Si1-yGey)2
Y. Tabata, S. Ohya, H. Taguchi, C. Kanadani, T. Taniguchi, H. Nakamura
Magnetic phase diagram under low temperature and high pressure in RVO3 II
D. Bizen, H. Nakao, K. Iwasa, Y. Murakami, T. Osakabe, S. Miyasaka, Y. Tokura
Magnetic-Field Variations of Antiferromagnetic Structure in CeRh1-xCoxIn5
M. Yokoyama, Y. Ikeda, I. Kawasaki, D. Nishikawa, K. Tenya, H. Amitsuka
Magnetic Excitations of LaFeAsO0.89F0.11
T. Moyoshi, S. C. Lee, A. Kawabata, Y. Kobayashi, Y. Yasui, M. Sato, K. Kakurai
Magnetic excitations of NaxCoO2.yD2O
T. Moyoshi, Y. Yasui, M. Sato, K. Kakurai
Fe-doping dependence of magnetic correlations in Bi2201
H. Hiraka, K. Yamada
Identification of an order parameter in a heavy fermion antiferromagnet CeTe3
K. Deguchi, N. Aso, H. Iwase, T. Okada, G. F. Chen, N. K. Sato, H. Yoshizawa
Thermal variations of magnetic excitation spectrum in slightly overdoped
Bi2.1Sr1.9CaCu2O8+δ
M. Matsuura, Y. Yoshida, H. Eisaki, N. Kaneko, C.-H. Lee, K. Hirota
Inelastic neutron scattering experiment on deuterated halogen-bridged nickel complex
S. Itoh, T. Yokoo
Electric Control of Helimagnetic Chirality in CoCr2O4
Y. Kousaka, M. Nishi, K. Tomiyasu, M. Matsuura, K. Hirota, T. Yokobori, J. Akimitsu
Mechanism of Spontaneous Electric Polarization Flop in TbMnO3
H. Sagayama, N. Abe, T. Arima, K. Iwasa
Thermoelectric properties and crystal structures in layered Co oxides
H. Nakatsugawa, K. Nagasawa
Thermoelectric properties and crystal structures in layered Co oxides
H. Nakatsugawa, K. Nagasawa
Nonmagnetic impurity effect in ferroelectric phase of CuFeO2
T. Nakajima, S. Mitsuda, M. Yamano, H. Yamazaki, M. Matsuura, K. Hirota
Magnetic Phase Diagram in Ba2Mg2Fe12O22
H. Sagayama, K. Taniguchi, T. Arima, Y. Nishikawa, S. Yano, J. Akimitsu, M. Matsuura,
K. Hirota
Magnetic Property of PrxFe4Sb12
K. Iwasa, T. Orihara, Y. Murkami, K. Kuwahara, H. Sugawara
Crystal-field excitation and multipolar ordering in Pr(Ru1 xRhx)4P12
K. Iwasa, K. Saito, L. Hao, Y. MurakamiElectric Field Control of Magnetic Correlation in Multiferric Cu(Fe,Al)O2
K. Takahashi, Y. Kaneko, T. Ito, T. Nakajima, S. Mitsuda
Rattling vibration of cage compounds
C. H. Lee, H. Yoshizawa, K. Kihou, T. Onimaru, K. Suekuni, T. Takabatake
Spin fluctuations of single-layer in Bi2+xSr2-xCuO6+d superconductor
M. Fujita, M. Enoki, K. Yamada
Dual structure in spin excitations of La2-xSrxCuO4 studied through impurity effectM. Fujita, M. Enoki, S. Iikubo, K. Yamada
Doping evolution of spin correlations in electron-doped Pr1-xLaCexCuO4
M. Fujita, J. Kaminaga, K. Yamada
Crystal structure of the calcium-ferrite type 1-D chain compounds CaCo2O4
M. Isobe, Y. Matsushita
Magnetic structure study of the multi-step metamagnet CeIr3Si2
Y. Muro, K. Motoya, K. Shigetoh, T. Takabatake
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- 10 -

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1-3-26 Competition between Hidden Order and Pressure-Induced Antiferromagnetism in URu2Si2
H. Amitsuka, Y. Ikeda, I. Kawasaki, S. Takayama, D. Nishikawa, M. Yokoyama
1-3-27 Quasi-elastic neutron scattering measurements on the kagome lattice
antiferromagnet KFe3(OH)6(SO4)2
K. Matan, T. J. Sato, D. Grohol, D. G. Nocera, Y. S. Lee- 11 -

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1-4-3
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1-4-9
1-4-10「 Title 」
Neutron Scattering -Amorphous ・ LiquidAnalogy on the Self-assembled Fractal-like Structure between the Niobate
Nanosheet Colloidal Solution and Block Copolymer Lamellar Morphology
D. Yamaguchi, N. Miyamoto, S. Koizumi, T. Nakato, S. Akasaka, M. I. Kim, H. Hasegawa,
T. Hashimoto
Hydrophobic hydration and partial molar volume of alcohol aqueous solutions
K. Maruyama, M. Nakada, M. Misawa
Hydration structure around the nitrogen atom of the pyridine molecule
Y. Kameda, A. Maki, Y. Amo, T. Usuki
DMF-induced Phase Separation of HFIP-Water Mixtures
T. Takamuku, T. Shimomura, M. Tachikawa
Alkyl-chain Dependence of Mixing State for Methanol Solutions of
Imidazolium-based Ionic Liquids
T. Takamuku, T. Shimomura, K. Fujii
Nano-scale aggregation structure formed in room temperature ionic liquid and its
application to the new reaction field
K. Fujii, T. Shimomura, T. Takamuku, Y. Umebayashi, S. Ishiguro
Temperature variation of the diffusional motion of water molecules in n-propyl
alcohol aqueous solution
K. Maruyama, M. Nakada, T. Kikuchi, C. Matsumoto, O. Yamamuro
Study on micro-solvent extraction mechanism using ionic liquid-water mixed
solvents by SANS
K. Fujii, S. Homi, T. Takamuku, M. Tabata
Structural investigation on super crtical CO2 and co-solvent system
M. Sugiyama, T. Sato, K. Ito, K. Mori, T. Fukunaga
QENS Studies of Fast Molecular Reorientation in Isotropic, Glass, Smectic, andCrystalline Phases of 6O2OCB
H. Suzuki, A. Inaba, J. Krawczyk, M. Massalska-Arodz, T. Kikuchi, O. Yamamuro- 12 -

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No.
1-5-1

1-5-2

1-5-3

1-5-4
1-5-5
1-5-6
1-5-7

1-5-8
1-5-9
1-5-101-5-11
1-5-12

1-5-131-5-141-5-151-5-16
1-5-171-5-181-5-19
1-5-201-5-21

1-5-22
1-5-23「 Title 」
Neutron Scattering - Polymer SANS Study of PEEK-Based Polymer Electrolyte Membrane Prepered by
Radiation-Induced Graft Polymerization
S. Hasegawa, S. Takahashi, H. Iwase, S. Koizumi, Y. Maekawa
Combined SANS, WANS, and Weighing Studies of Microbial Cellulose:
Elucidation of Hierarchical Structures in Drying Process
Y. Zhao, S. Koizumi, T. Hashimoto
Effect of Dynamic Nuclear Polarization on Small Angle
Neutron Scatterings of Diblock Copolymer with a Lamellar Structure
Y. Noda, T. Kumada, T. Hashimoto, S. Koizumi
Gel structure with excess water in a surfactant solution
Y. Kawabata, A. Matsuno, T. Shinoda, T. Kato
Structure characterization of Tetra-PEG gel having homogeneous network structure
T. Sakai, T. Matsunaga, M. Shibayama, U. Chung
Dispersion Stability of Carbon Black Suspensions by the Addition of Polymers
M. Kawaguchi, H. Mizukawa, Y. Takahashi
Study on Structural Nonuniformity of Cross-linked Natural Rubber
Y. Ikeda, N. Higashitani, H. Asai, Y. Kokubo, T. Suzuki, N. Osaka, H. Endo, M. Shibayama,
S. Kohjiya
Structure and compressibility of worm-like lamellar domain in a hydrated solid phase
Y. Kawabata, T. Shinoda, Y. Nagai, A. Murakami, T. Kato
Shear-induced onion formation of complex bilayer membrane systems
S. Fujii, Y. Kawabata, Y. Takahashi
Small Angle Neutron Scattering Study on Metal-containing Gels Composed of
Co(II) Ion and Oligopyridines
J. Yoshida, S. Nishikiori, T. Matsunaga, M. Shibayama
Breathing Mode in Polymer Micelles and Second Virial CoefficientK. Kawashima, T. Kanaya, G. Matsuba, H. Endo
Distribution of Glass Transition Temperature Tg in a Polymer Thin Film by Neutron
Reflectivity
K. Kawashima, T. Kanaya, G. Matsuba, K. Nishida, M. Hino
Role of Low Mw Components in Polymer Crystallization under Shear Flow
C. Ito, G. Matsuba, K. Nishida, T. Kanaya
Neutron Scattering Study on Miscibility of Statistical Copolymer / Homopolymer BlendsSiti Sarah A. R., D. Kawaguchi, Y. Matsushita
Dynamical Properties of Nanoporous Structure in Syndiotactic Polystyrene
F. Kaneko, T. Kawaguchi, K. Okuyama
Static/Dynamic Structural Investigation of Lipid Nanodiscs
M. Nakano, M. Fukuda, M. Miyazaki, Y. Wada, H. Endonano-meter-sized domain formation in model bio-membrane
Y. Sakuma, M. Imai
Neutron Reflectivity Studies of the Swelling States of Polysulfobetaine Brush at
Water Interface
Y. Terayama, M. Kobayashi, A. Takahara
Structure-Property Relationship of Particle-Polymer Mixture Solution under shear field
M. Shibayama, T. Matsunaga, T. Suzuki, N. Osaka, T. Nishida, H. Endo
Kinetic process on transition from small to large uni-lamellar vesicles
N. L. Yamada
Structural Analysis of N-isopropylacrylamide / Rod-like silica Hybrid Gels by
Contrast-variation Small-angle Neutron Scattering
T. Suzuki, N. Osaka, H. Endo, M. Shibayama
Structural Analysis of Polyurethane Resin by Small-angle Neutron Scattering
T. Suzuki, M. Shibayama, K. Hatano, M. Ishii
Small-angle neutron scattering study of block copolymers in supercritical carbon dioxide
M. Itoh, H. Yokoyama, K. Mayumi, K. Ito, N. Osaka, H. Endo, M. Shibayama- 13 -

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1-5-24 Reconstruction of uni-lamellar vesicles induced by addition of polymers
N. L. Yamada
1-5-25 Relation between bending modulus and spontaneous curveture in DGI/SDS/D2O system
H. Mayama, X. J. Chen, M. Nagao, H. Seto, K. Tsujii
1-5-26 Conformation and Dynamics of Polyrotaxane in Solution
K. Mayumi, H. Endo, N. Osaka, H. Yokoyama, M. Shibayama, K. Ito
1-5-27 Mechanically Interlocked Structure of Polyrotaxane Investigated by Contrast
Variation Small Angle Neutron Scattering
K. Mayumi, H. Endo, N. Osaka, H. Yokoyama, M. Shibayama, K. Ito
1-5-28 QENS Study on Thermal Gelation in Agarose Aqueous Solution
N. Onoda-Yamamuro, O. Yamamuro
1-5-29 Aggregation Structure and Dynamics of Polymers at the Interface with Water I:
Analysis of Aggregation Structure by Neutron Reflectivity
H. Atarashi, T. Nagamura, M. Hino, K. Tanaka
1-5-30 Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: II. Analysis of Relaxation Dynamics by Neutron Spin Echo
H. Atarashi, T. Nagamura, K. Tanaka, H. Endo, M. Shibayama
1-5-31 An Effect of Electromagnetic Wave Treatment on Polymer Diffusion
H. Atarashi, T. Nagamura, M. Hino, K. Tanaka
1-5-32 Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: I. Analysis of Aggregation Structure by Neutron Reflectivity
H. Atarashi, T. Nagamura, M. Hino, K. Tanaka
1-5-33 Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: I. Analysis of Aggregation Structure by Neutron Reflectivity
H. Atarashi, T. Nagamura, M. Hino, K. Tanaka
1-5-34 Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: II. Analysis of Relaxation Dynamics by Neutron Spin Echo
H. Atarashi, T. Nagamura, K. Tanaka, H. Endo, M. Shibayama
1-5-35 Large scale structure and crossover of critical phenomena induced by solvation effect
H. Seto, K. Sadakane, N. Iguchi, H. Endo
1-5-36 Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: I. Analysis of Aggregation Structure by Neutron Reflectivity
H. Atarashi, T. Nagamura, M. Hino, K. Tanaka
1-5-37 An Effect of Electromagnetic Wave Treatment on Polymer Diffusion
H. Atarashi, T. Nagamura, M. Hino, K. Tanaka
1-5-38 Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: II. Analysis of Relaxation Dynamics by Neutron Spin Echo
H. Atarashi, T. Nagamura, K. Tanaka, H. Endo, M. Shibayama- 14 -

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「 Title 」

Neutron Scattering - Biology Hydration Level Dependent Protein Dynamics Studied by Neutron Inelastic Scattering
H. Nakagawa, M. Kataoka
1-6-2 Neutron Diffraction Study of Porcine Pancreatic Elastase under Active Conditions
T. Tamada, T. Kinoshita, T. Ohhara, K. Kurihara, T. Tada, R. Kuroki
1-6-3 Contrast Variation Measurements of Various Intermediates of Hen Egg White
Lysozyme Amyloid Fibrils
S. Fujiwara, F. Matsumoto, H. Nakagawa
1-6-4 Small-Angle Neutron Scattering Measurements of Rhodanase-GroEL-GroES Complex
K. Ichimura, Y. Matsuura, S. Fujiwara, Y. Kawata, H. Kihara
1-6-5 Neutron Diffraction of Protein Single Crystals in H2O
S. Fujiwara, T. Ohhara, T. Chatake
1-6-6 Enhancement of Lipid Flip-Flop by Membrane Proteins and Transmembrane Peptides
M. Nakano, M. Fukuda, M. Miyazaki, Y. Wada, H. Endo
1-6-7 Structure and dynamics of β-lactogloblin in alcohol-water mixture
K. Yoshida, T. Yamaguchi
1-6-8 Effect of temperature and pressure on protein dynamics studied by inelastic
neutron scattering
H. Nakagawa, Y. Joti, O. Yamamuro, M. Kataoka
1-6-9 Denaturation of alpha-Crystallin by replacement of amino-acid residue
M. Sugiyama, N. Fujii, T. Fukunaga, N. Fujii
1-6-10 Analysis of the relationship between the dynamics and the structuralpolymorphism of F-actin
S. Fujiwara, F. Matsumoto, H. Nakagawa, T. Oda
1-6-1- 15 -

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No.
1-7-1
1-7-2
1-7-3

Neutron Scattering - Fundamental Physics ・ Neutron Optics Development of Neutron Interferometer using polychromatic mirrors
M. Kitaguchi, M. Hino, Y. Seki, H. Funahashi, K. Taketani, H. M. Shimizu
Measurement of magnetic diffuse scattering from Ni2MnAl
K. Hayashi, K. Ohoyama, T. Yamamoto, T. Shishido
A study on reｆｌectivity limit of neutron supermirror
M. Hino, M. Kitaguchi, H. Hayashida, T. Ebisawa, R. Maruyama, N. Achiwa, Y. Kawabata「 Title 」

No.

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1-8-2

1-8-3
1-8-4
1-8-5
1-8-6
1-8-7

1-8-8
1-8-9

1-8-101-8-11

1-8-12

1-8-131-8-141-8-151-8-161-8-17

3

Develpoment of U-shaped He PSDs for DNA,A New Backscattering Spectrometer at J-PARC
N. Takahashi, K. Shibata, T. Yokoo, S. Satoh, K. Nakajima
Effect of Interfacial Roughness Correlation on Diffuse Scattering Intensity
in a Neutron Supermirror
R. Maruyama, D. Yamazaki, T. Ebisawa, K. Soyama
Performance Test of Scintillator-based Small Neutron Detector
K. Sakasai, T. Nakamura, K. Toh, A. Moriai, E. Shooneveld, N. Rhodes
Measurement of Energy Spectrum of Neutron Beam at MUSASI-H Port
K. Toh, H. Yamagishi, K. Sakasai
Development of a Multiplet Magnetic Lens System to Focus a Pulsed Neutron Beam
T. Oku, H. Kira, T. Shinohara, S. Takata, M. Arai, J. Suzuki, H. M. Shimizu
Neutron Beam Focusing with a m= 4 Supermirror on a Precisely Figured Elliptic Surface
D. Yamazaki, R. Maruyama, K. Soyama, H. Takai, M. Nagano, K. Yamamura
Development of a Wavelength-Shifting-Fibre-Based Neutron Imager With a
Fibre-Optic-Taper With a High Spatial Resolution
T. Nakamura, M. Katagiri, K. Toh, K. Sakasai, S. Soyama
Development of the Rradiation-resistant Neutron Mirrors for Neutron Guides
I. Tamura, R. Maruyama, D. Yamazaki, K. Yamamoto, K. Soyama
Development of a Hybrid-Anvil Type High-Pressure Device for Single-Crystal
Magnetic Neutron Diffraction under 10 GPa
T. Osakabe, H. Yamauchi
Renewal of a Software and a Data Acquisition System
for the Neutron Reflectometer SUIREN
M. Takeda, D. Yamazaki, H. Izunome, A. Birumachi
A beam divergence correction mirror for neutron resonance spin echo
R. Maruyama, M. Hino, H. Hayashida, M. Kitaguchi, N. Achiwa, D. Yamazaki, T. Ebisawa,
K. Soyama
Development of Cubic Anvil type pressure cell for neutron scattering experiments
under pressure
K. Munakata, K. Matsubayashi, M. Nishi, H. Kagi, Y. Uwatoko
Development of resonance spin flipper with iron yoke
M. Kitaguchi, M. Hino, Y. Kawabata, S. Tasaki, H. Hayashida, R. Maruyama, T. Ebisawa
Magnetic Imaging with Neutron Spin Interferometry
D. Yamazaki, H. Hayashida, T. Ebisawa, R. Maruyama, K. Soyama, N. Takenaka, M. Kageyama,
S. Tasaki, M. Hino, Y. Kawabata, H. Iikura, R. Yasuda, T. Sakai, M. Matsubayashi
A new MIEZE technique for investigation of relaxation on magnetic nanoparticles
M. Hino, H. Hayashida, M. Kitaguchi, N. Achiwa, Y. Kawabata
Development of Cubic Anvil type pressure cell for neutron scattering experiments
under pressure
K. Munakata, K. Matsubayashi, M. Nishi, Y. Uwatoko
Development of pixel detector for ultra-cold neutrons
Y. Kamiya, S. Kawasaki, G. Ichikawa, S. Sonoda, S. Komamiya, M. Hino, M. Kitaguchi,
T. Sanuki- 16 -

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1-9-2

No.

「 Title 」
Neutron Scattering - Superconductivity Structural Analysis on Fe-Based Superconductors, PrFeAsO1−xFx and PrFeAsO1−y
K. Kodama, M. Ishikado, F. Esaka, A. Iyo, H. Kito, H. Eisaki, S. Shamoto
Magnetic Excitations in LaFeAsO1−xFx Superconductors
S. Wakimoto, K. Kodama, M. Ishikado, M. Matsuda, R. Kajimoto, M. Arai, K. Kakurai,
A. Iyo, H. Kito, H. Eisaki, S. Shamoto「 Title 」

Neutron Scattering - Residual Stress 1-10-1 Behavior of Crack Growth of Austenitic Stainless Steels under Decrease in Stress
H. Ogawa, I. Ioka, M. Yamamoto
1-10-2 Stress Measurement of Large Scaled Welded Tube Using Neutron Diffraction Technique
H. Suzuki, J. Katsuyama, T. Tobita, Y. Morii
1-10-3 Strain Measurement in Rebar in Reinforced Concrete by Neutron Diffraction
H. Suzuki, K. Kusunoki
1-10-4 Relaxation of Residual Stress in Engineering Component
K. Akita
1-10-5 Residual Stress Measurement of Thick Butt Weld Using Neutron Diffraction
H. Suzuki, J. Katsuyama, Y. Morii
1-10-6 Development of Cryogenic Load Frame for Neutron Diffraction
H. Suzuki, Y. Tsuchiya, T. Umeno, S. Machiya, K. Osamura
1-10-7 Development of Multi-channel Vertical Conversing Slit
H. Suzuki, Y. Shinohara, T. Oku, J. Suzuki, M. Hayashi
No.

「 Title 」

Neutron Scattering - Others 1-11-1 Anomalous Lattice Dynamics in Relaxor K1−xLixTaO3
S. Wakimoto, H. Taniguchi, G. A. Samara, R. K. Grubbs, E. L. Venturini, L. A. Boatner
1-11-2 Neutron diffraction experiments of valence fluctuating YbPd
A. Mitsuda, M. Sugishima, K. Ohoyama, H. Wada
1-11-3 Structural Evaluation of Titanate Nanotube and Nanosheet
A. Nakahira, T. Kubo, M. Yashima- 17 -

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3-14
3-15
3-16

「 Title 」
Neutron Radiography
Development of the Very High-Frame-Rate and High Resolution Neutron Radiography System
for High Speed Multi-Phase Flow Visualizations
M. Kureta
Development of Multi-pinhole Collimator for Large Imaging Area with High spatial Resolution
H. Hayashida, M. Segawa, R. Yasuda, H. Iikura, T. Sakai, M. Matsubayashi
Evaluation of Spatial Resolution in Computed Tomography Images used Single
Aperture Devices in Thermal Neutron Radiography Facility in JRR-3
H. Iikura, R. Yasuda, H. Hayashida, T. Sakai, M. Matsubayashi
Visualization of Water Behavior in an Operating Fuel Cell
H. Iikura, R. Yasuda, T. Sakai, M. Matsubayashi, Y. Katada
Investigation of Distribution and Diffusion of Hydrogen and Lithium in the Electrode andElectrolyte Materials for All-Solid State Rechargeable Batteries
H. Sakaguchi, T. Esaka, M. Nanjo, S. Takai, T. Iida, M. Matsubayashi, H. Iikura「 Title 」
Neutron Activation Analyses
Revealing volcanotectonic history of Philippine Sea region using 40Ar/39Ar dating method
O. Ishizuka, A. Matsumoto
Mössbauer spectroscopic studies of inorganic compounds Part VI
M. Takahashi, T. Ayabe, S. Tokita, T. Numano, Y. Hirai, T. Misu, K. Imai
Measurement of Hyperfine Field of a Metal Site of Proteinby the Method of Perturbed Angular Correlation of Gamma-Rays
A. Yokoyama
Study of Hyperfine Field using Low-temperature Nuclear Orientation
S. Ohya, T. Ohtsubo, T. Izumikawa, S. Muto, K. Nisimura
Sensitive detection of alkaline cryptotephra layers in deep-sea cores from the Sea of Japan
using high-resolution INAA analysis
K. Toyoda, C. Lim, A. Umetsu, N. Kawashima, Y. Shinozuka, M. Nitanai
Luminescence dating of eustatic sediments and annual dose measurements by NAA
Y. Ganzawa
Arsenic and antimony contents in the Setouchi Volcanic Rocks
H. Shinjoe
Activation analysis of river, estuarine and marine sediments
M. Matsuo, A. Kuno, K. Shouzugawa, A. Hasegawa, D. Moromachi, A. Takahashi,
S. Yamanoi, M. Hoshino, T. Yamano, N. Hara, M. Fujii
Thermochronological study of rocks in the orogenic belts II
H. Hyodo, T. Itaya, C. Gouzu
Production identification method of consumer products including ores as radiation sources andclassification of ores by Sm/Gd ratios.
E. Furuta, H. Minowa
Determination and behavior of trace elements in atmospheric samples (Ⅱ)
T. Honda, K. Hirose, Y. Kikawada
Effects of Zn deficiency on metalloproteins in hepatic and pancreatic cells
M. Yanaga, H. Suganuma, M. Noguchi, J. Kamishima, M. Kawashima, W. Muramatsu,
Y. Yamano, T. Kawaguchi, A. Kawamura, H. Shimoyama, O. Yamamoto
Environmental Investigation of Metallic Elements by Dendrochronology with Activation Analysis
Y. Katayama, M. Nagai, T. Aoki, N. Okada, Y. Kawabata
Instrumental Neutron Activation Analysis of Halogen in Coral Skeletons
S. Ohde, K. Tanaka
Dynamics of biotrace elements in selenium deficient female and male rats
K. Endo, C. Honda, K. Matsuoka, M. Tsukada
Aluminum Analysis in Biological Materials by Instrumental Neutron Activation Analysis
Y. Katoh, Y. Yamamoto- 18 -

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3-18

3-19
3-20
3-21

No.
4-1

A growth depending uptake of some rare metal into Clethraceae leaves
S. Kasahara, Y. Noya, K. Seki
Elemental Compositions of Atmospheric Suspended Particulate Matters
by PGA and INAA (II)Y. Oura, M. Ebihara, T. Tomita, S. Sugawara, T. Suzuki, T. Otoshi
Prompt Gamma-ray Analysis of Boron in Marine Carbonates
S. Ohde, K. Tanaka
Study on the new encapsulated-fullerenes using radiochemical method
K. Sueki, Y. Iwai, M. Tamari, K. Akiyama
Determination of trace elements in old iron and tea leaves as environmental standard
candidate by neutron activation analysis
S. Hirai, M. Kato, Y. Okada「 Title 」
OthersSelective detection of particles containing highly enriched uranium for nuclear safeguards
environmental samples
C. G. Lee, K. D. Suzuki, F. Esaka, M. Magara, S. N. Shinohara, S. Usuda- 19 -

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1.  ୰ ᛶᏊᩓ஘ 1 ᵓ㐀࣭ບ☢ 
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1. Neutron Scattering

1 Structure࣭Excitation- 21 -

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JAEA-Review 2013-039

1-1-1
Phonon Dispersion Relations of LaAlO3 -SrTiO3
H. Yamauchi, T. Shimada1 , K. Ichikawa1 , J. Breeze2 and N. McN Alford2
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
Advanced Electronics Research Laboratory, Hitachi Metals, Ltd., Kumagaya, Saitama 360-0843
2
London South Bank University, London SE1 0AA, UK

The SrTiO3 doped LaAlO3 (LAO-STO)
has the pseudo-cubic perovskite structure. It
has been expected to apply single crystal
LAO-STO in dielectric resonators and electromagnetic ﬁlters because of extremely low
dielectric loss at microwave communications
frequencies1) . However, it is known that its
loss is strongly depend on whether the incident direction of electromagnetic wave isalong [1 0 0] or [1 1 0]2) . Predicting the dielectric loss in applicative materials at microwave frequency band has generally turned
out to be highly problematic, though it isvaluable for material developers to possess themeans of the preliminary prediction. Sparket al. proposed that two-phonon absorption
process between transverse acoustic (TA) andoptic (TO) modes at the Brillouin zone (BZ)
boundary is mainly important for dielectricloss in the microwave region3, 4) .

cept for the TO mode and a part of the TA
modes in q  [1 1 0]. The energy gap between
the TA and TO modes at the BZ boundary is 18.3 meV in q  [1 0 0] and 13.7 meVin q  [1 1 0]. Comparing theoretical prediction of losses with direct measurements is notstraightforward because theories assume perfect (defect- and impurity-free) single crystals. Theories, however, have prospects ofproviding a lower limit for the intrinsic dielectric loss. In the future, we will examine theavailability of the theoretical method for predicting dielectric loss in LAO-STO as a candidate of the applicative materials.

In order to collect the fundamental phonon
dispersion data, we therefore carried out
inelastic neutron scattering experiments atroom temperature using the triple-axis spectrometer TAS-1. The single crystal sample of
1.5 mol% SrTiO3 doped LaAlO3 was used forexperiments. Measurements were performedin the constant-Q mode with incident neutronenergies of 14.7 – 41.0 meV. The scattering
was carried out in a net plane of (h k k ).
Figure 1 shows the dispersion curves forphonons with wave vectors along [1 0 0] and[1 1 0] directions. The markers denote the experimental data. The calculated dispersion
curves of LaAlO3 with cubic symmetry arealso shown as reference by the dashed lines.
The open circles and triangles correspond to
TA and TO phonon modes, respectively. The
closed circles stand for longitudinal acoustic
modes. The experimental results are largely
consistent with the calculated dispersion ex原子炉：JRR-3

装置：TAS-1(2G)Figure 1: Phonon dispersion curves for 0.985 LaAlO3 0.015 SrTiO3 . The dashed lines represent the calculation of phonon dispersion relation in LaAlO3 .

References
1) T. Shimada et al., J. Eur. Ceram. Soc. 26, 2017(2006).
2) T. Shimada et al., J. Eur. Ceram. Soc. 25, 2901
(2005).
3) M. Spark et al., Phys. Rev. B 26, 6987 (1982).
4) X. Aupi et al., J. Appl. Phys. 95, 2639 (2004).

分野：中性子散乱（構造）- 23 -

JAEA-Review 2013-039

1-1-2
Crystal Structure and Nuclear Density Distribution of LiCo1/3 Ni1/3 Mn1/3 O2
Analyzed by Applying Rietveld/Maximum Entropy Method
N. Igawa, T. Taguchi, H. Fukazawa, H. Yamauchi, and W. Utsumi
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

原子炉：JRR-3

装置：HRPD(1G)

Figure 2 shows the scattering length density
distribution maps of LiCo1/3 Ni1/3 Mn1/3 O2
drawn with the absolute values of isosurface
level, a)1.0 fm/Å3 and b)0.05 fm/Å3 . While
the scattering length density distributions ofCo, Mn, Ni, and O atoms were localized attheir sites, those of Li atoms at z =0, 1/3 and2/3 widely spread on the planes parallel to(0001) plane.
10000

8000

6000

Intensity

LiCo1/3 Ni1/3 Mn1/3 O2 is one of the candidate materials for cathode of next generation
Li ion batteries. In general, the crystal structure and Li diﬀusion pathway are the keys toincrease eﬃciency for the battery. Recently
maximum entropy method (MEM) combinedwith neutron powder diﬀraction has been extensively used to investigate the crystal structures of ionic conductors, because MEM is effective for revealing static and dynamic disorder in crystals. In this study, we analyzed
the nuclear density (scattering length density)
distribution of LiCo1/3 Ni1/3 Mn1/3 O2 by Rietveld and MEM analysis of neutron powder
diﬀraction data to estimate the Li diﬀusing
pathway.
The sample was prepared by a solid state
reaction method. We used 7 Li enriched LiOH
as a starting material to suppress the adsorption of neutron beam. Neutron powder
diﬀraction measurements were carried out atroom temperature using the HRPD. A neutron wavelength of 0.1823 nm was used. Crystal structure was determined from the diﬀraction pattern by the Rietveld method using the
program RIETAN-FP .1) After the Rietveld
analysis, the scattering density distribution
map was estimated by applying the maximum
entropy method analysis using the program
PRIMA .2)
Figure 1 shows a result of Rietveld reﬁnement. All peaks were from the sample and noreﬂections of impurities were observed. The
R wp , R B and S are 4.28 %, 1.66 % and 1.19.
LiCo1/3 Ni1/3 Mn1/3 O2 has a hexagonal structure with the space group R-3m. Lattice parameters were reﬁned to be a = 2.8643(2) Å,c = 14.2460(6) Å. Though Li mainly occupies
3a site, Co, Ni and Mn occupy 3b site, andO 6c site, approximately 4 % of Li and Ni
atoms substitute from their original sites (3aand 3b) to 3b and 3a sites.

4000

2000

0

20

30

40

50

60

70

80

90

2

100 110 120 130 140 150 160/°

Figure 1: The result of the Rietveld analysis of
LiCo1/3 Ni1/3 Mn1/3 O2 .

Figure 2: Scattering length density distribution maps.

References
1) F. Izumi et al.:“Solid State Phenom.”, 130:15(2007).
2) F. Izumi et al.:“Recent Research Development inPhysics II”, 3, 699(2002).

分野：中性子散乱（構造）- 24 -

JAEA-Review 2013-039

1-1-3
Neutron Powder Diﬀraction Study of Water-Dissolved Ba2 In2 O5
T. Nagasaki1 , S. Shiotani2 , M. Yoshino2 , K. Iwasaki2 ,N. Igawa3 , H. Fukazawa3 , H. Yamauchi3 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

In our previous studies 1, 2) , we carried out
neutron powder diﬀraction experiments on
BaSn0.5 In0.5 O2.75 , a proton conducting oxidewith perovskite structure, with and without
dissolved H2 O/D2 O. Analyzing the data by
the Rietveld method and the maximum entropy method (MEM), we found that the deuterium atoms in BaSn0.5 In0.5 O2.75+α were located at the 48n site close to the 12h site of
the cubic perovskite structure (space groupPm3m).

cordingly we have tested larger unit cells withlower symmetry, but not yet obtained satisfactory ﬁts to the observed patterns. Further
study is needed.

In the present study, we have carriedout similar experiments on another proton conducting oxide Ba2 In2 O5 , which hasperovskite-derivative (brownmillerite) structure.
Because of its lower symmetry,
Ba2 In2 O5 has various interstitial sites, someof which must be more stable than others forhydrogen.
Figure 1(a) shows the diﬀraction pattern of(dry) Ba2 In2 O5 at 8 K. Although it was wellﬁtted by the orthorhombic (Imma) structure
model 3) , there remained a few small peaks
that could not be assigned. In fact, these
extra peaks were also seen in the reported
diﬀraction patterns 3, 4) . Because they disappeared after water uptake 4) , they are unlikely
to be caused by impurities.
Figure 1(b) and (c) show the diﬀraction
patterns for Ba2 In2 O6 H2 and Ba2 In2 O6 D2 at
8 K, respectively. While the Rietveld ﬁtting
based on the tetragonal (P4/mbm) structure
model 5, 6) gives a reasonable ﬁt for the protonated material, it gives a poor ﬁt for the
deuterated material. Provided that the isotope eﬀect in the crystal structure is negligible, this result suggests that the actual atomic
arrangement especially of hydrogen is diﬀerent from that in the structure model. Ac原子炉：JRR-3

装置：HRPD(1G)

Figure 1: Neutron powder diﬀraction patterns at 8 Kof (a)Ba2 In2 O5 , (b)Ba2 In2 O6 H2 , and (c)Ba2 In2 O6 D2 ,together with the results of Rietveld ﬁtting (diﬀerenceplots) using RIETAN-FP.

References
1) T. Ito, T. Nagasaki et al. :“Solid State Ionics”,
178, pp. 607-613 (2007).
2) T. Nagasaki et al. :“J. Solid State Chem.”, inpress (2009).
3) P. Berastegui et al. :“J. Solid State Chem.”, 164,
pp. 119-130 (2002).
4) T. Yildirim et al. :“Solid State Ionics”, 145, pp.
429-435 (2001).
5) V. Jayaraman et al. :“Solid State Ionics”, 170, pp.
25-32 (2004).
6) J.-R. Martinez et al. :“J. Solid State Chem.”, 180,
pp. 3388-3392 (2007).

分野：中性子散乱（構造）- 25 -

JAEA-Review 2013-039

1-1-4
Structure of Ice XI and a New Form, Ice XV
H. Fukazawa
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Ice is the major solid component in the universe. By infrared space observatory (ISO),ice has been founded in many locations frominterstellar clouds to planets, their satellites
and Kuiper belt objects. The infrared spectra have a strong peak at around 3.08 micro
meter, which assigned to OH stretching vibration in crystal ice. The observed crystal
ice in space is generally cooled below 80 K.
According to the third low of thermodynamics and Pauling’s ice rules, the hydrogen in
crystal ice should be ordered at very low temperature. Thus frigid ice in space may be not
ice Ih but hydrogen-ordered ice. The ordered
ice is named ice XI (eleven). A hypothesisthat ice XI exists in the Universe is reported[1-7].
We measured neutron powder diﬀraction(NPD) and infrared (IR) absorption spectraof doped ice samples with impurities, in orderto understand the properties of ice in space.
NPD shows that the hydrogen is ordered in
ice and the resulting solid becomes ferroelectric ice XI (eleven). The ferroelectric ice isstable in wide range of temperature and pressure. IR spectra of ice XI have sharp peaks inlibrational and OH stretching modes.
Ferroelectric high-pressure ice, named ice
XV, has long been predicted to exist above
0.7 GPa and below 160 K. We made ice XV at
1 GPa and 70 K on the HRPD using a highpressure cell (McWhan type cell of alumina
powder developed by Prof. Onodera) and top
loading cryostat. In this march we have obtained the diﬀraction proﬁle of ice XV at 1
GPa, which has a new peak (2.37 angstrom)from hydrogen-ordered structure. The proﬁleis consistent with a ferroelectric structure.
Our preliminary study suggests that a new
ice XV is also ferroelectric. Thus large quantities of ferroelectric ice should exist on icy
bodies in outer solar system. The propertiesof ferroelectric ice are of interest in space be原子炉：JRR-3

装置：HRPD(1G)

cause of long-range electrostatic force. The
ferroelectricity becomes very important feature for planetary formation and material(including life origin material) evolution in
space. A plan (ISO by a space telescope) toprove this hypothesis is proposed [8].
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 RD 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).
6) H. Fukazawa :“J. Crystallog. Soc. Jpn”, 51, pp.
84-85 (2009).
7) H. Fukazawa et al. :“Nucl. Instrum. Methods Phys.
Res. A”, 600, pp. 279-281 (2009).
8) M. Arakawa, et al. :“Astrophys. J.”, in press.

分野：中性子散乱（構造）- 26 -

JAEA-Review 2013-039

1-1-5
Correlation Eﬀects among Thermal Displacements of Atoms in KBr
T. Sakuma, Xianglian, N. Shimizu, J. Yokokawa, 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

Correlation eﬀects among thermal displacements of atoms are important to realize thethermal properties of materials1) . The oscillatory diﬀuse scattering intensities were observed from ordered crystals at room temperature due to the correlation eﬀects among
thermal displacements of atoms2) . The valuesof correlation eﬀects decrease rapidly with theincrease of inter-atomic distance.
The correlation eﬀects among thermal displacements of atoms are also obtained by EXAFS analysis. The value of the correlation effects of 1st nearest neighboring atoms in KBr
was very small compared to other ionic crystals. We discuss the inter-atomic distance andtemperature dependence of correlation eﬀects
in KBr by neutron diﬀraction method.
Neutron diﬀraction measurements were
performed on powder KBr at 7 and 295 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 KBr are shown bysolid lines (295K) and broken lines (7K) in
Fig. 1.
The diﬀuse neutron scattering proﬁle of
KBr at room temperature was explained by
the correlation eﬀects among thermal displacements of atoms up to third neighboring
atoms. The value of correlation eﬀects among
1st nearest neighboring atoms in KBr (0.68)
by diﬀuse neutron scattering measurement isgreater than that (0.4) by EXAFS measurement. When we calculate the diﬀuse scattering intensity with the value 0.4, the oscillatory
feature of the calculated intensity is very weakcompared with that of the observed neutron
diﬀuse scattering intensity.
原子炉：JRR-3

装置：HRPD(1G)

The force constant is related to correlationeﬀects and Debye-Waller temperature parameters. The phonon dispersion relation is calculated by the force constants among atoms.
The force constant of ﬁrst nearest neighboring atoms is obtained by EXAFS measurement, whereas the force constants of ﬁrst, second and third nearest neighboring atoms are
obtained by the analysis of diﬀuse scattering. Therefore we would estimate the phonon
dispersion relation from the analysis of diffuse scattering intensity by X-ray and neutron diﬀraction measurements with a highaccuracy than the method of EXAFS measurement. The derivation of phonon dispersion relation from the correlation eﬀects is inprogress.

Figure 1: Neutron scattering intensities of powder
KBr.

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）- 27 -

JAEA-Review 2013-039

1-1-6

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2&&*-,-y&[n^0`#x&].1!12-.e!Za*X¬­®¯$ggXh °±¯3fX$^WhXn` ²³¯´µ­¶·¸¹º»- 28 -

JAEA-Review 2013-039

1-1-7
Nano-structure analysis of high Cr steel for long life FBR structural material
S. Obara1 , J. Suzuki2 , T. Wakai1 , S. Ohtsuka1 , M. Inoue1 and T. Asayama1
1Core and Structural Materials Group, Advanced Nuclear System RD Directorate
2
Materials and Life Science Division, J-Parc Center

For the commercialization of fast breeder reactor (FBR), it is essential to reduce construction
cost by employing high chromium (Cr) steels as
main structural materials. The conventional highCr steels which have been developed as the materials for thermal power boilers have both excellent high temperature strength and thermal
properties, such as thermal conductivity and thermal expansion rate. Generally, high temperature strength of the high Cr steels is achieved byseveral strengthening mechanisms. Precipitation
strengthening mechanism by ﬁne precipitations,such as V(C,N), Nb(C,N) and Cr23 C6 , is the mostimportant one. In this study, in order to estimate
the precipitation strengthening eﬀect in high Cr
steel, the size distribution and number density ofﬁne precipitations were estimated using transmission electron microscope (TEM) and small angle
neutron scattering (SANS) analyzer. In addition,
the relationship between high temperature properties and number density of ﬁne precipitations wasevaluated based on the mechanical test results andmicrostructural observations.
In order to estimate the size distribution andnumber density of ﬁne precipitations, V and Nb
added high Cr steel was prepared. Chemical compositions of the steel are 0.1C-10Cr-1.2Mo-0.12V0.03Nb-0.05N-Fe (mass%). The steel were normalized at three diﬀerent temperatures, namely
1060˚C, 1100˚C and 1150˚C for 1 hour, and thentempered at 760˚C for 1 hour. The TEM observation was performed using extracted replicas specimen. The SANS analyses were performed in the q
range of 0.01〜1 (nm−1 ) using SANS-J-II in JRR3, and the nuclear scattering information was obtained by applying one-directional magnetic ﬁeldof 1 (Tesla) to the specimens.
The shape, distribution and chemical compositions of ﬁne precipitations were investigated using TEM observations. Then, the size distribution
and number density of ﬁne precipitations were obtained from the measured SANS proﬁles and TEM
observations. The inﬂuence of normalizing temperature on the size distribution of ﬁne precipitations obtained from SANS analyses is shown in
Figure 1. The mean diameter of ﬁne precipitations decreased with increase of normalizing temperature, and the number density became lager

原子炉：JRR-3

装置：SANS-J(C3-2)

with increase of normalizing temperature. Figure
2 shows the relationship between high temperature strength and normalizing temperature. Both
0.2% proof stress and ultimate tensile strength
increased with increase of normalizing temperature. Number density of ﬁne precipitations also
described in Figure 2, there is a good correlation
between high temperature strength and number
density of ﬁne precipitations. These results showthat SANS analyses and TEM observations canevaluate size distribution and number density ofﬁne precipitations which correlated with high temperature strength of high Cr steel.

Figure 1: Inﬂuence of normalizing temperature on size
distribution of ﬁne precipitations in high Cr steel.

Figure 2: High temperature strength and number density of ﬁne precipitations versus normalizing temperature.

分野：中性子散乱（構造）- 29 -

JAEA-Review 2013-039

1-1-8
Development of High Pressure Device for Neutron Powder Diﬀraction− Feasibility Test using Lanthanum Hydride −W. Utsumi, T. Hattori, A. Machida1 and N. Igawa
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Quantum Beam Science Directorate, JAEA, Sayo, Hyogo 679-5148

1

In situ powder diﬀraction with x-rays or
neutrons is an indispensable technique to investigate the structure of materials underhigh pressure. For neutron diﬀraction, various high-pressure experiments have previously been conducted at nuclear reactors andwith pulsed neutron sources. Further rapid
progress is expected owing to the opening of
J-PARC. Development of high pressure device
suitable for neutron diﬀraction has been madeusing the High Resolution Powder Diﬀractometer (HRPD) at JRR-3.
A Paris-Edinburgh press was mounted on
the rotation stage of HRPD. A pair of toroidal
anvils made of tungsten carbide (WC) wasused for the pressure generation. Diﬀraction
proﬁles of Lanthanum hydride (LaHx ) powder (initial size: 5mm in diameter and 2.5mm
in height) placed in the high pressure cellwere observed at 3.5 GPa (applied load: 37
ton). Lanthanum hydride has been studied
intensively because it exhibits metal-insulatortransition upon hydrogenation and various
phase transition occurs under high pressure.

Incident and diﬀracted neutron beams (wavelengh:1.823 °A) pass through the anvil gap
which is perpendicular to the compression
axis. The exposure time was 37 hours.
Figure 1 shows the diﬀraction proﬁles at 3.5
GPa. Nine peaks of LaHx were clearly observed together with those from WC anvils.
Although there are still many problems to besolved such as reduction of background andprecise intensity measurements, feasibility ofneutron powder diﬀraction under high pressure was conﬁrmed. Using this high pressuredevice, the ﬁrst high experiment was carriedout at J-PARC (BL19), and the diﬀraction
proﬁles of standard sample (Pb) were successfully obtained.
References
1) W.Utsumi, H.Kagi, K.Komatsu, H.Arima, T.Nagai,
T.Okuchi, T.Kamiyama, Y.Uwatoko, M.Matsubayashi
and T.Yagi, Nucl.Instr.Meth.Phys.Res.A 600, 50(2009).

Figure 1: Diﬀraction proﬁles of LaHx at 3.5 GPa.

原子炉：JRR-3

装置：HRPD(1G)

分野：中性子散乱（構造）- 30 -

JAEA-Review 2013-039

1-1-9
Study of Mesoscale Spatial Distribution of Electron Spins in High Crystallinity
Polyethylene Doped with TEMPO Using Time-Resolved Dynamic Nuclear
Polarization and Small-Angle Neutron Scattering Methods
T. Kumada, Y. Noda, S. Koizumi, T. Hashimoto
Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195

We studied the mesoscale spatial distribution of the electron spins in the highcrystalline polyethylene (PE) doped with
TEMPO radicals by means of combined timeresolved dynamic nuclear polarization (DNP)
and small-angle neutron scattering (SANS).
DNP results from transferring spin polarization from electrons to nuclei, thereby aligning
the nuclear spins to the extent that the electron spins are aligned. Proton spins at theneighbor of the electron spins are dynamicallypolarized by DNP. Since scattering length ofa polarized neutron against a proton remarkably depends on relative direction of theirspins, the scattered pattern of the polarized
neutron reﬂects the spatial distribution of the
proton polarization. The idea is that the spatial distribution of the electron spins can be
determined by the SANS measurement of the
distribution of the polarization generated by
DNP.
We implemented the technique of double
microwave-frequency DNP system and timeresolved SANS system. The DNP system enables to generate positive and negative proton polarization by switching the microwave(MW) frequency. The time-resolved SANS
measures the spatial distribution of the polarization as a function of time after the switching of MW.
Figure 1 shows SANS proﬁles of the dynamically polarized PE. The scattering intensity
at q ≤ 0.02 Å measured 1 min after the stwiching of MW is larger than that measured ≥ 10
min after the switching and that of the unpolarized sample, whereas intensity of the peakat q = 0.02 Å−1 was much less changed.
High crystallinity PE has lamellar structurecomposed of crystalline (C) and amorphous(LA) phases, which generates the peak at q =0.02 Å−1 , whereas the regions other than the
原子炉：JRR-3

装置：SANS-J(C3-2)

lamellar are amorphous (AA). It was found byelectron spin resonance study that TEMPO is
localized in the LA and AA regions but notin the C region. We speculate that the polarization at the AA region grew faster thanthat at the C and LA regions. The remarkable increase in the scattered intensity measured 1 min after the switching is expected
to be due to the diﬀerence in polarization between the lamellar and the other regions. The
small change in the peak intensity at q = 0.02
Å−1 suggests that the spin diﬀusion between
C and LA is too fast to observe their diﬀerence in polarization within the time-scale ofmeasurement.

Figure 1: SANS proﬁles of dynamically polarized highcrystallinity PE doped with TEMPO measured at 3.3
T and 1 K.

分野：中性子散乱（構造）- 31 -

JAEA-Review 2013-039

1-1-10High Temperature Neutron Diﬀraction Study of (La0.5Sr0.5)CoO3-d Perovskite
K. Nomura (A), H. Kageyama (A), K. Kakinuma (B), T. Maekawa (C), S. Nakamura(C),H. Miyazaki (C), H. Imabayashi (C), T. Ito (C), and M. Yashima (D)(A) AIST, (B) Yamanashi University, (C) New Cosmos Electric Co., Ltd., (D) Tokyo Institute ofTechnology
Recently, strontium-doped lanthanum
cobaltate perovskites, (La1-xSrx)CoO3-dhave been investigated as the cathode materials of solid oxide fuel cells, because of
the high electronic and high oxide-ion conductivity [1]. However, the detailed crystal
structures under cell operation conditions,
i.e., at elevated temperatures under oxygen
partial pressures, P(O2)<=0.21atm, havenot been reported yet. In this study, we
have measured high temperature neutron
diffraction data of 50 mol% Sr-doped
LaCoO3, (La0.5Sr0.5)CoO3-d (LSC), atelevated temperatures, 298<=T<=1273K,
under 0.0002<=P(O2)<=0.21atm, to investigate the detailed crystal structures.
Neutron diffraction measurements were
performed 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 2 θ =0.1 deg. A furnace with Pt-Rh heaters installed in a vacuum chamber was placedon the sample stage, and used for neutrondiffraction measurements at high temperatures under different P(O2) conditions. The
diffraction data obtained were analyzed using the Rietveld program RIETAN-2000 [3].
The diffraction data of LSC could be indexed assuming a trigonal symmetry (R3c, No.167) between 298 and 608K, or a
cubic one (Pm-3m, No.221) between 723
and 1273K under P(O2) = 0.21atm. Almost all the diffraction peaks could be indexed as a tetragonal system (P4/mmm,
No.123) at 1073K in P(O2) = 0.0002atm.
Figure 1 shows the Rietveld reﬁnement result of LSC measured at 1273K in P(O2) =0.0004atm. Under this condition, almost all
the diffraction peaks could be indexed asa cubic perovskite phase (Pm-3m, No.221)(In addition, trace amount of CoO phase
was detected). The reﬁned cell parametersof perovskite phase were as follows: Z = 1, a
= 3.9395(3)A, α = 90 deg., V = 61.138(8)Aˆ3.
The reliability factors were Rwp = 5.81%,
RI = 3.93%, RF = 2.14%, and Re = 2.12%.
Goodness of ﬁt (S = Rwp/Re) was 2.73.
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(La0.5Sr0.5)CoO3-d at 1273K in P(O2) = 0.0004 atm.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 673- 32 -

JAEA-Review 2013-039

1-1-11

Structural Disorder and Diﬀusional Pathway of Oxide Ions in a Doped
Pr2NiO4-Based Mixed Conductor
Masatomo Yashima, †,* Makiko Enoki, ‡ Takahiro Wakita, † Roushown Ali, ¶, †Yoshitaka Matsushita, ¶ Fujio Izumi, ¶ Tatsumi Ishihara ‡† Department of Materials Science and Engineering, Interdisciplinary Graduate School of
Science and Engineering, Tokyo Institute of Technology, Nagatsuta-cho 4259, Midori-Ku,
Yokohama, Kanagawa 226-8502, Japan, ‡ Department of Applied Chemistry, Faculty ofEngineering, Kyushu University, Motooka 744, Nishi-Ku, Fukuoka, Fukuoka 819-0395, Japan,and ¶ Quantum Beam Center, National Institute for Materials Science, 1-1 Namiki, Tsukuba,
Ibaraki 305-0044, Japan
Mixed oxide-ionic and electronic conducting ceramics (MIECs) are attracting muchinterest as materials for oxygen separation membranes. Oxygen can permeate
through MIECs membranes when a gradient of oxygen chemical potential exists.
A2BO4-based oxides with K2NiF4-type
structure have extensively been studied
as new mixed ionic-electronic conductors,
where A and B are cations. The development of improved MIECs requires a better
understanding of the mechanism of ionic
conduction, and crucial to this is a comprehensive knowledge of the crystal structure.
It was speculated that the oxide ion conduction in the A2BO4-based oxides occurs
by diffusion of excess oxide ions along therock-salt-type AO layers. However, thediffusion path of oxide ion has not been
determined yet. Pr2NiO4-based oxides
have high oxygen permeability and highdiffusivity of oxide ions. Here, we reportfor the ﬁrst time the diffusion path of oxideions in a K2NiF4-type mixed conductor(Pr0.9La0.1)2(Ni0.74Cu0.21Ga0.05)O4+d(PLNCG), through a high-temperatureneutron powder diffraction study (M.
Yashima, M. Enoki, T. Wakita, R. Ali,
Y. Matsushita, F. Izumi and T. Ishihara,
Structural Disorder and Diffusional
Pathway of Oxide Ions in a Doped
Pr2NiO4-Based Mixed Conductor , J. Am.
Chem. Soc. (Communications), 139, [9]2762-2763 (2008).). We chose this chemicalcomposition, because it exhibits high oxygen permeability. The present result would
give hints for the design of K2NiF4-typeconductors.
A PLNCG sample was prepared by asolid-state reaction method at 1300 oC for
6 h in air. Neutron powder diffraction
data of PLNCG were in situ measured
at 606.6 oC and 1015.6 oC using a furnace and a 150 detector system HERMES.
at a neutron wavelength of 1.82646
Neutron diffraction patterns at both temperatures indicated a K2NiF4-type structure with I4/mmm space group. Neutrondiffraction data were analyzed by a combination of Rietveld analysis, the maximumentropy method (MEM), and MEM-based
pattern ﬁtting (MPF). A computer program RIETAN-2000 was utilized for the Rietveld analysis and MEM-based whole pattern ﬁtting, and VESTA for visualization of
nuclear density (scattering-length density)
distribution. It is known that MPF makes it
possible to determine nuclear densities incompounds containing disordered chemical species from neutron diffraction data.
Rietveld reﬁnements of the neutron diffraction data of PLNCG at 606.6 oC and 1015.6
oC were successfully performed on thebasis of the K2NiF4-type structure with
I4/mmm space-group symmetry. It was
found that PLNCG has a crystal structure
consisting of (Ni,Cu,Ga)O6 octahedron and(Pr,La)-O layers. Reﬁned occupancy factors
indicated the excess oxygen of d = 0.0154(3)in (Pr0.9La0.1)2(Ni0.74Cu0.21Ga0.05)O4+
d, which is ascribed to the interstitial O3
atom. The O3 atom is located at a 16n
site, i.e., (x, 0, z) where x = 0.666(19)and z = 0.223(9) at 1015.6 oC. The oxy-

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 687- 33 -

JAEA-Review 2013-039

gen atom at the O2 site (4e; (0, 0, z); z= 0.1752(4) at 1015.6 oC) exhibits highly
anisotropic thermal motion (U11 = U22 =0.115(3) 2 and U33 = 0.021(3) 2), whichleads to the migration of oxide ions to thenearest-neighbor interstitial O3 positions.
The striking feature in the nuclear density distribution is the curved O2-O3 diffusion path. This feature is ascribed to therepulsion between (Pr,La) and O atoms.
In fact, the distance between the (Pr,La)
and O atoms are kept approximately constant along the diffusion paths. This factsuggests that the large-sized cations suchas Pr and La ions at the A site in theA2BO4-type conductor are effective in improving the oxide-ionic conduction on the
A-O layer. The conduction path is alongthe <100> directions near the O2 site
and roughly along the <301> directions
around the center of the paths. The nucleardensity distribution also shows the twodimensional (2D) network of the O2-O3O2 diffusion paths of oxide ions. The 2Dfeature is consistent with the anisotropictransport of oxide ions in La2NiO4+d. The
nuclear density on the diffusion path at
1015.6 oC is larger than that at 606.6 oC,
which is consistent with the improved oxygen permeability at higher temperatures.

1-1-11- 34 -

JAEA-Review 2013-039

1-1-12

Neutron diﬀraction study of Yb compounds
M.Kurisu, H.Murakami, 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
The interesting phenomenon of zero thermal expansion has been recently reported
to occur in a wide temperature range from100 to 300 K in YbGaGe compound [1]. The
anomalous thermal expansion is caused by
the decrease of Yb ion radius associatedwith valence ﬂuctuation with increasing
temperature. Because the temperature dependence of the effective magnetic moment
calculated from the result of susceptibility measurement indicated that the valenceof the Yb ion varies from 2+ to 3+. However, the experimental result was shown tosuggest that the YbGaGe compound is diamagnetic [2]. Therefore, a correlation between valence ﬂuctuation and zero thermal
expansion has been doubted.
Furthermore, as for the thermal expansion anomaly that this compound showed,
its sample dependence was large. A lot ofquestions do not yet reach solution about
presence and cause of zero thermal expansion in the YbGaGe compound.
The purpose of this study is to examine
the zero thermal expansion in the YbGaGe
compound experimentally.

The powder neutron diffraction pattern at
300 K is shown in Figure 1. The anisotropic
thermal expansion was observed. The analysis is in progress.

References[1] J. R. Salvador, F. Guo, T. Hogan and M.
G. Kanatzidis: Nature 425(2003) 702.
[2] Y. Muro, T. Nakagawa, K. Umeo, M.
Itoh, T. Suzuki and T. Takabatake: Journalof the Physical Sociey of Japan 73 (2004)
1450.

Fig. 1. The powder neutron diffraction pattern of
YbGaGe at 300 K

The single phase polycrystalline samples of YbGaGe compound was preparedby melting the constituent elements in atetra-arc furnace under a Ti-gettered highpurity argon atmosphere. The measurement of thermal expansion of bulk samples was performed with differential transformer and strain gage methods. The powder neutron diffraction was carried out inthe temperature range from 10 to 300 K
at neutron beam-line T1-3 of JRR-3M at
Tokai. Rietveld method was employed forthe analysis. Heat capacity was measured
with a PPMS.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 697- 35 -

JAEA-Review 2013-039

1-1-13

Measurement of over dumped phonon on protonic conductor K3 H(SeO4 )2
F. Shikanai1 , S. Itoh2 , K. Tomiyasu3 , N. Aso4 , T. J. Sato4 , S. Ikeda2 and T. Kamiyama2
1 Univ. Tsukuba, 2 IMSS-NSL KEK, 3 IMR, Tohoku University, 4 ISSP-NSL Univ. Tokyo
Protonic conductor K3 H(SeO4 )2 undergoes ﬁrst order phase transition at 390 K(TC , 385 K on the cooling process), andshows high electric conductivity above TC .
We have measured the inelastic neutron
scattering (INS) of the material, and observed a broad spectrum around 0 meV atzone boundary L-point above TC . Intensityof the spectrum increases with decreasing
the temperature, and the spectrum is considered to be caused by an over dumped
phonon. However, quantitative nature of
the spectrum was unclear because of thenarrow shape of the spectrum less than the
resolution. We, therefore, performed an energy scan from −0.2 meV to 0.2 meV undera possible high resolution within the scattering condition. The ﬁnal momentum vector kf was ﬁxed at 1.39 Å−1 . The energy
resolution was estimated as 88(3) μeV fromthe FWHM of incoherent scattering of hydrogen under a collimation of G-Be-20 -S40 -Be-40 .
Figure 1 shows the temperature dependence of INS spectrum at L-point subtracted incoherent scattering which obtained at 0.7 2 0. The broad peak was observed only at L-point, therefore, the spectra are caused by an coherent scattering
having the same symmetry of rotational
SeO4 tetrahedra. To analyze the data in
Fig. 1, a equation formulated for neutron
scattering cross section by over dumped
phonon [1] was used. The equation was
simpliﬁed as ATγ{( T − T0 + BΔq2 )( E2 +γ2 )}−1 with the four parameters A, B, T0and γ. The results of ﬁtting substituted
Δq = 0 for the ﬁtting function are illustrated as the plane in Fig 1. As shownin the ﬁgure, the data are good agreementwith the calculated plane. The extrapolated Curie temperature T0 was obtained
as 368(2) K. The parameter γ was assumed
as a linear function of T obtained from ﬁt-ting at each temperature using a normal
Lorentz function, as shown in the inset ofFig 1. The FWHM of the spectrum, 2γ,
slightly depends on the temperature, andis obtained as 60(4) μeV and 70(6) μeV at
386 K and 435 K, respectively. This energy
range corresponds to 14(1) GHz and 17(1)GHz, and gives the lifetime from 7.1(4) ×
10−11 s to 5.9(4) × 10−11 s. Although it isexpected that the lifetimes are little longer
then this result because of the resolution,
this time scale agrees with the stationary
time of conduction proton, 9.0(8) × 10−11
s at 388 K and 4.9(3) × 10−11 s at 433 K, obtained from quasi elastic neutron scattering(QENS) [2]. It shows that proton conduction is simultaneous with the motion of rotational mode in phase I.
References[1] Y. Yamada et al.: Phys. Rev. 177 (1969)848.
[2] F. Shikanai et al.:Ferroelectrics 347(2007)74.

Fig. 1. Temperature dependence of INS spectra at
L-point (subtracted incoherent scattering).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 698- 36 -

JAEA-Review 2013-039

1-1-14

Phonon dispersion of oﬀ-stoichiometric Ni2 MnGa sigle crystal
K. Inoue A , Y. YamaguchiB , H. HirakaB
A Advanced Research Institute for Science and Engineering, Waseda University, B IMR, Tohoku
University
Inelastic neutron scattering experiments
were used to study an off-stoichiometric
Heusler-type Ni2.16 Mn0.78 Ga1.06 single
crystal. A triple-axis neutron spectrometer,
AKANE, was used. The alloy has a martensitic transformation temperature aroundroom temperature (293 K) coincident witha Curie temperature. It is ferromagnetic
in the martensitic phase and paramagnetic
in the mother phase and is expected asa magnetic-ﬁeld-induced shape memory
alloy. With decreasing temperature thealloy transforms from a cubic structure toa metastable orthorhombic structure andﬁnally to a stable tetragonal structure.1)
Diffraction patterns of the cubic structure and of the orthorhombic structure
projected on the reciprocal cubic c*-plane
are shown in Figs. 1(a) and (b). At 400
K the alloy shows a cubic structure andat 279K it shows an orthorhombic one.
In the orthorhombic structure at 279 K,
we see several elastic diffuse scatterings
along the〈110〉and〈100〉directions of
the orthorhombic c*-plane and many weaksatellite peaks on these diffuse scatterings.
These diffuse scatterings and the satellite
peaks appear to show that the lattice ismodulated to various extent along〈110〉and〈100〉directions.
TA2 -phonon dispersions with〈110〉and〈100〉propagations in the cubic phasewere measured at several temperatures.
As shown in Figs. 1(c) or (d), the softeningof the phonon is observed at q=0.3 or at
q=0.23, respectively. The softening of thephonon with〈110〉propagation is explicitly temperature dependent. However, thetemperature dependence of the softeningof the phonon with〈100〉propagation is
not clear. Near the position in the q-spacecorresponding to the softening of theTA2 -phonon dispersion, the elastic satellite

peaks in the metastable orthorhombic
structure appear. Thus, the softening of theTA2 -phonon in the mother phase appears
to be a precursory phenomenon to themetastable martensitic structure.
1) K. Inoue, Y. Yamaguchi, H. Hiraka, et.
al.: J. Phys. Soc. Jpn. 78 (2009) 034602.

Fig. 1. (a), (b) Elastic q-mesh scans on the reciprocal lattice cubic c*-plane at 400 and 279 K, (c),(d) TA2 -phonon dispersions with cubic〈110〉and〈100〉propagations.

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JAEA-Review 2013-039

1-1-15Structure and Magnetism of Inﬁnite Layer Iron Oxide with a Square-Planar
Coordination
Tassel C., Tsujimoto Y., Kageyama H., Yoshimura K., Takano M., Nishi M., Ohoyama K.
Kyoto University, University of Tokyo, Tohoku University
The coordination geometries more usuallyexhibited by iron in oxides are octahedraland tetrahedral.1 However the use of calcium hydride as a low-temperature reductant, a technique recently introduced by
Hayward, Rosseinsky and coworkers, hasprovided a way to circumvent this structural choice. For instance, Tsujimoto et al.
have recently reported a new material, SrFeO2, in which a high-spin Fe2+ exhibitsa square-planar coordination. This material is build from unprecedented FeO2 inﬁnite layers in between which the Sr2+
cations reside (see Fig. 1(left)) and exhibits a number of surprising structuraland physical properties. The study of theelectronic structure of SrFeO2 has provided
important clues to understand this situation. Later, this material was shown to beremarkably robust towards cation substitution and temperature6 opening the way towards possible applications. More recently
the same technique was used to preparea new spin-ladder iron oxide, Sr3Fe2O5,
which again exhibits high-spin Fe2+ ions ina square-planar coordination.

to well-studied and accepted concept thatoctahedral rotation in perovskite oxides occurs but the octahedral shape is kept almost regular.
[1] T. Cedric et al., J. Am. Chem. Soc. 131,
221-229 (2008).

Fig. 1. Crystal structures of the ideal inﬁnite structure SrFeO2 (left) and the distorted one CaFeO2(right).

The neutron diffraction study and the synchrotron X-ray diffraction revealed that
CaFeO2 exhibit an unprecedented layered
structure [1]. The new phase was obtained through a low-temperature reduction procedure using calcium hydride. The
XAS spectra near the Fe-K edge for thewhole solid solution (Sr1-xCax)FeO2 supports that iron is in a square-planar coordination for 0 < x < 0.8 but clearlysuggests a change of coordination for x= 1. The new structure contains inﬁnite
FeO2 layers in which the FeO4 units unprecedentedly distort from square-planar
toward tetrahedra and rotate along the caxis (see Fig. 1(right)), in marked contrast
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1-1-16

Observation of the spin gap in a two-dimensional quantum spin system(CuCl)Ca2Nb3O10
Tsujimoto Y., Kageyama H., Yoshimura K., Ajiro Y., Nishi M.
Department of Chemistry, Graduate School of Science, Kyoto University; Institute for Solid
Staet Physics, University of Tokyo
Low-temperature syntheses may offer promising routes to innovate lowdimensional
magnetic
compounds,
as metastable solids. Indeed, reacting
a double-layered nonmagnetic DionJacobson phase RbLaNb2O7 with CuX2
yields a perovskite/metal halide intergrowth structure (CuX)LaNb2O7 (X = Cl,Br), where the interlayer Rb+ ions are replaced by the [CuX]+ layer with an S = 1/2
square lattice. We have recently reported
that the ground state of (CuCl)LaNb2O7
is described by the quantum spin liquid,
where no long-range order exists down to
20 mK and the spin-singlet ground stateis separated from the triplet excited statesby a gap of 2.3 meV. On the other hand,(CuBr)LaNb2O7 has a spin order at 32
K, with a spin structure of the so-called
collinear (pi, 0) type. We then exploredthe triple-layered system (CuX)A2B3O10
which is expected to have an enhanced
two-dimensionality as the magnetic CuXlayer in the triple-layered system is separeted by the perovskite slab as long as
16 angstrom, 1.5 times longer than the
double-layered case. (CuBr)Sr2Nb3O10
showed a quantized magnetization plateau
corresponding to the 1/3 of the fully saturated magnetization for Cu. The stabilityof the 1/3 plateau can be controlled bysubstituting A and B site with Ca, Ba, Pb,
and with Ta, respectively.
In this study, we investigate a series of(CuCl)A2B3O10 compouds. From the magnetic susceptiblity and magnetization measurements, the spin singlet nature with aﬁnite gap to the ﬁrst excited triplet stateis suggested in (CuCl)Ca2Nb3O10. It follows that this compound provides thegood comparison to (CuCl)LaNb2O7. Inorder to directly probe the existence ofthe singlet-triplet excitations and to understand the spin-singlet formation mechanism, we performed the inelastic neutron
scattering study using two spectrometers at
JRR-3, 5G and C1-1.
As shown in Fig. 1, we successfully observed the singlet-triplet excitations ataround 1.5 meV, obtained at C1-1. The obtained spin-gap value agrees well with thegap estimated from the magnetic susceptibility and speciﬁc heat measurements. The
Q-dependence of this excitation shows afast oscillation behavior, as in the case of(CuCl)LaNb2O7, and a simple dimer picture gives the dimer distance as long as 8
angstrom, which is physically unlikely.

Fig.
1.
Singlet-triplet(CuCl)Ca2Nb3O10

excitationsinActivity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-17

Behavior of Thermal Parameters and the Phase Transition in DKDP
H. Mashiyama A , T. Miyoshi A , T. Asahi A , H. KimuraB , Y. NodaB
A Fac. Sci. Yamaguchi Univ., B IMRAM Tohoku Univ.
It has been considered that the tunneling character of proton is coupled withother heavy atoms to induce ferroelectricity below 123 K in KDP (KH2 PO4 ). If protons are replaced by deuterons, the transition temperature elevates up to Tc =213 K in DKDP. There remains a question whether heavy atoms are in disorderedor displacive within anharmonic potentials
above Tc . In order to elucidate this point,
we have performed detailed structure analyses of DKDP above and below Tc .
Single crystals were grown by evaporation method from a heavy water solution of DKDP powder provided commercially. A rectangular prism of 2.8 × 2.6 × 2.5mm3 was cut from a transparent block of
the crystal. Aluminum electrodes were attached on the c-planes to apply an electricﬁeld so that the crystal was single domain
below Tc . Neutron diffractmeter FONDER
was employed to collect diffracted intensity data. Measured temperatures were10, 70, 120, 160, 190, 210, 223, 250 and
303 K. Every proﬁles of the reﬂection peaks
were checked and programs DABEX andRADIEL were used to correct absorption
and extinction effects. Crystal structures
were reﬁned by using the least squaredcalculation program, SHELXL-97. Split
atom method was employed to represent
disordered character of deuteron above
Tc . All data sets were successfully analyzed; the R factors were about 4 % withanisotropic thermal parameters.
The positional parameters are almost
steady below Tc . Figure 1 (a) displays thetemperature dependence of the dipole moment of the unit cell estimated by assigning
simple ionic point charges to each atom.
The values are almost in good agreementwith the reported spontaneous polarization (Samara 1973). All the Debye-Waller
factors (mean-squared displacement) U33

decrease monotonically with decreasing
temperature as shown in Fig. 1 (b). They
do not vanish even at 0 K, representing
quantum zero-point vibration, whose magnitude is lower than the expected value
from the room temperature phase (Nelmes
et al. 1982).
Below Tc , the ordering of deuteron induces a distortion of PO34− tetrahedron anda displacement of K+ ion. The magnitudes of the thermal vibration of K and P
changes little at Tc . If they are disorderedunits in the paraelectric phase, they shouldhave greater thermal parameters. So it ishard to image a disordered P or K above
Tc . The thermal parameter indicates that D
is almost in the ground state below 100K.
A comparison with KDP will be presented
elsewhere.

Fig. 1. Temperature dependence of (a) the estimatedpolarization with K+ , D+ , P5+ and O2− , and (b) the
Debye-Waller factor U33 .

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JAEA-Review 2013-039

1-1-18Correlation between crystal defects and the diﬀuse scattering in relaxor
ferroelectric (Na0.5 Bi0.5 )TiO3
M. Matsuura1 , K. Hirota1 , Y. Noguchi2 , and M. Miyayama2
1 Department of Earth and Space Science, Faculty of Science, Osaka University, Toyonaka,
560-0043.
2 Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo
153-8505
Relaxor ferroelectrics have attracted considerable attention since the discovery of
giant piezoelectricity in relaxor-based single crystals. (Na0.5 Bi0.5 )TiO3 (NBT) forms
perovskite structure with two different ions
Na+ and Bi3+ at the A-site of ABO3 . A
key-concept to understand the relaxor behavior is polar nanoregion (PNR), a local nanometer-sized region with ferroelectric polarization and atomic shift. Such an
atomic shift in PNR was observed for a typical relaxor such as PMN and PZN as characteristic diffuse scattering. In NBT, wehave revealed anisotropic diffuse scattering which extends along 110-directions.
Recently, Noguchi et al. succeeded in suppressing Bi-defects in NBT single crystal byhigh O2 -pressure, and found larger polarizations than those in the crystal grown inair.[1] The purpose of the present work is
to compare the diffuse scattering in crystals
grown in different O2 pressure to clarify thecorrelation between the diffuse scatteringand ferroelectric properties. Neutron scattering experiments were performed on the
triple-axis spectrometers HQR installed at
the JRR-3 Guidehall of JAEA.
Figure 1 shows proﬁles of (h, 1, 0) scanmeasured at room temperature. At T ∼300 K, large diffuse scattering appears
around (110) and extends along 110directions. In order to compare diffuse
scattering quantitatively, scattering intensities are normalized by sample mass. Proﬁles consist of sharp peak of (110) Bragg
reﬂection and broad peak of diffuse scattering. Apparently, the diffuse scatteringfor O2 -10 atm crystal is smaller than thatfor O2 -0.2 atm crystal. From previous measurement, we found that this anisotropic

diffuse scattering shows large temperaturedependence and appears strongly alongtransverse direction, which suggests close
correlation between the diffuse scatteringand ferroelectric ﬂuctuations. Since number of Bi-defects is expected to be smaller in
O2 -10 atm crystal than O2 -0.2 atm crystal,the current results indicate that the diffuse
scattering, in other words, PNR are pinned
ferroelectric ﬂuctuations at crystal defects.
References[1] Y. Noguchi et al., Jpn. J. Appl. Phys. 47(9B),
7623 (2008).

Fig. 1. Proﬁles of (h, 1, 0) scan for NBT single crystals
grown in air (black circles: O2 0.2 atm) and high O2
pressure (red circles: O2 10 atm).

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JAEA-Review 2013-039

1-1-19Temperature dependence of waterfall feature of phonons in (Na0.5 Bi0.5 )TiO3
M. Matsuura1 , K. Hirota1 , Y. Noguchi2 , and M. Miyayama2
1 Department of Earth and Space Science, Faculty of Science, Osaka University, Toyonaka,
560-0043.
2 Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo
153-8505
Relaxor ferroelectrics have attracted considerable attention since the discovery of
giant piezoelectricity in relaxor-based single crystals. (Na0.5 Bi0.5 )TiO3 (NBT) forms
perovskite structure with two different ions
Na+ and Bi3+ at the A site of ABO3 . Recently, NBT regains attention as promising
applications to piezoelectric devices containing no toxic lead. Last year, we studied the lattice dynamics in NBT and clariﬁed so-called waterfall feature, anomalous
damping of transverse optic (TO) phonons
for reduced wave vector less than qw f =0.2Å−1 , which was commonly observed intypical lead-containing relaxors as PMN[1]and PZN-8%PT[2]. For PMN, it has beenshown that the recovery of TO mode occurs in ferroelectric phase and at very
high temperatures[3]. The purpose of thepresent work is to study temperature dependence of waterfall feature in detail andto conﬁrm recovery of TO mode. Neutron
scattering experiments were performed on
the triple-axis spectrometers PONTA installed at the JRR-3 Reactor hall of JAEA.
Figure 1 shows proﬁles of constant-E
scan along transverse direction from (220).
Inset shows the TA and TO dispersions at
T = 670 K, where no propagating mode
was observed for q < 0.10 rlu, and the
TO branch drops like waterfall to the TAbranch. Constant-E scan at E = 11 meV,
represented as the red arrow in inset,
crosses the waterfall TO branch and shows
peak at q = 0.16 rlu at T = 700 K. Withdecreasing temperature, the peak shifts towards Γ-point, and eventually disappears
at T = 300 K, which indicates disappearance of waterfall feature and recovery of
TO mode at T = 300 K. Actually, we observed TO mode at ω = 15 meV at Γ-

point for T = 300 K (not shown). Hlinka
et al. proposed that the waterfall feature
is explained by coupled damped TA and
TO modes[4]. The current result indicatesthat such coupling is universal in relaxors
and plays an important role in formation of
PNR.
References[1] P. M. Gehring et al., Phys. Rev. Lett. 87
277601 (2000).
[2] P. M. Gehring et al., Phys. Rev. Lett. 84 5216
(2000).
[3] S. Wakimoto et al., Phys. Rev. B., 65 172105(2002).
[4] J. Hlinka et al., Phys. Rev. Lett., 91 107602(2003).

Fig. 1. Proﬁles of constant-E scan of (2 − q, 2 + q, 0)with ﬁxed energy transfer of 11 meV. The data at
different temperatures are plotted with offsets.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-20Study of slow lattice dynamics in relaxor PMN-30%PT by neutron spin echo
techniqueM. Matsuura1 , H. Endo2 , and K. Hirota1
1 Department of Earth and Space Science, Faculty of Science, Osaka University, Toyonaka,
560-0043.
2 Institute for Solid State Physics, The University of Tokyo, 106-1 Shirakata, Tokai, 319-1106
Relaxor ferroelectrics are characterized
by a giant piezoelectricity associated withsigniﬁcant frequency dispersion. The variation of the diffuse maximum of the dielectric constant in wide frequency range gives
evidence for an important role of slow dynamics. A key-concept to understand therelaxor behavior is slowly relaxing polar
nanoregion (PNR), a local nanometer-sized
region with ferroelectric polarization andatomic shift. Such an atomic shift in PNR
was observed for a typical relaxor suchas PMN and PZN as characteristic diffuse
scattering. However, there is no decisive
understanding of the microscopic mechanism of the PNR formation at present. In
addition, recent neutron spin-echo measurement concluded that the diffuse scattering is purely elastic and is not related topolarization ﬂuctuations[1]. The purposeof the present work is to reinvestigate theintrinsic energy width of the diffuse scattering and clarify its mechanism. Neutron
spin-echo experiments were performed on
the iNSE installed at the JRR-3 Guide-hallof the JAEA. The sample was a high-quality
PMN-30%PT single crystal with a volumeof 1cc grown at JFE Mineral. The data
were taken with incident neutron energies
of 3.38 meV which enables access to diffuse
scattering near Q =(100) at 2θ = 74.5 degree.
Figure 1 shows the normalized intermediate scattering functions of the diffuse scattering at Q =(0.98, 0.02, 0) measured at various temperatures.
Below
T = 400 K, the normalized intermediate scattering functions I ( Q, t)/I ( Q, 0) do
not decay, which is associated with thelong-range ordered ferroelectric phase for
T < TC = 400 K. Note that the aver-aged I ( Q, t)/I ( Q, 0) are less than 1, indicating fast relaxations even in the orderedphase. At T = 450 K, I ( Q, t)/I ( Q, 0) is
ﬂat as T ≤ 400 K, but it drops from 0.9
to 0.6, suggesting enhancement of fast relaxations above TC . This is consistent withenhancement of meV-range broad quasielastic scattering at high temperatures[2].
Above T = 500 K, the I ( Q, t)/I ( Q, 0) has
maximum at 0.5 ns. Assuming this peak is
the ﬁrst peak of oscillation, it corresponds
to excitation of 4 μeV. This ultra-low energy mode may be related to the ferroelectric ﬂuctuations in PNR. Further study ishighly required to clarify the nature of thismode.
References[1] S. Vakhrushev, A. Ivanov, and J. Kulda,
Phys. Chem. Chem. Phys. 7 2340 (2005).
[2] H. Hiraka et al., Phys. Rev. B, 70 184105(2004).

Fig. 1. Normalized intermediate scattering functions I(Q,t)/I(Q,0) of the diffuse scattering at (0.98,
0.02, 0).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-21

Pseudospin-phonon coupling in Relaxor Ferroelectrics PMN-x%PT
M. Matsuura and K. Hirota
Department of Earth and Space Science, Faculty of Science, Osaka University, Toyonaka,
560-0043.
Relaxor ferroelectrics gain much attention due to their extreme piezoelectric responses over a wide temperature range. It
is widely believed that polar nanoregion(PNR), a local nanometer-sized region withferroelectric polarization and atomic shift,plays an important role in the relaxor behavior. Despite intense investigations, themicroscopic mechanism of the formation of
PNR remains unclear. The structural phasetransition are usually divided in displacement or of order-disorder type. From neutron scattering, soft mode was reported,suggesting displacement behavior[1]. On
the other hand, quasi-elastic scattering has
also been reported, which indicates orderdisorder mechanism. This coexistence reminds pseudospin-phonon coupled system
which was studied thoretically by Y. Yamada et al.[2] and conﬁrmed experimentally by Y. Noda[3]. The purpose of thepresent work is to clarify the nature ofpseudospin-phonon coupling in relaxors.
Neutron scattering experiments on typicalrelaxor ferroelectrics PMN-30%PT single
crystal were performed on the triple-axis
spectrometers HER installed at the JRR-3
Guide-hall of the JAEA.
Figure 1 shows the contour map of
the phonon scattering intensity at (1 +q, 1 − q, 0) measured at T = 400 K. At
T = 400 K(∼ TC ), the transverse acoustic (TA) mode below 2.5 meV is heavily
overdamped, while the TA mode above
2.5 meV is underdamped.
This overdamping starts from T ∼ 500 K on cooling. In the pseudospin-phonon coupledsystem, phonon becomes overdamped oncooling to TC when phonon frequency iscomparable to the relaxation rate of spinﬂipping. On the other hand, underdamped
spectrum is expected for higher frequency
phonon modes than the relaxation mode.

Current result indicate that relaxors is theintermediate case between displacive andorder-disorder type due to strong coupling
between relaxations (Γ ∼ 2.5 meV) of polarization in PNR and phonon modes.
References[1] P. M. Gehring et al., Phys. Rev. Lett., 87,
277601 (2001).
[2] Y. Yamada et al., J. Phys. Soc. Jpn, 36 641(1974).
[3] Y. Noda et al., J. Phys. Soc. Jpn, 48 1576
(1980).

Fig. 1. The contour map of the phonon scattering
intensity at (1 + q, 1 − q, 0) as a function of q and energy measured at T = 400 K. The line of color shows
intensity from 5 counts (blue) to 1000 counts (red).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-22Crystal structure analysis in pressure-induced commensurate magnetic phase ofmultiferroic HoMn2 O5
H. Kimura1 , Y. Sakamoto1 , T. Yamazaki1 , Y. Noda1 , N. Aso2 , T. Fujiwara3 , K.
Matsubayashi4 and Y. Uwatoko4
1 IMRAM, Tohoku University, 2 Ryukyu University, 3 Department of Physics, Yamaguchi
University, 4 ISSP, The university of Tokyo
HoMn2 O5 is well known as multiferroics showing colossal magnetoelectric effect. We have reported recently
that hydrostatic pressure induces theincommensurate–commensurate magnetic
phase transition[1], which leads to the
induction of large electric polarization[2].
This indicates the strong relevance between
the magnetic structure and ferroelectricity.
It was thought that the minute changeof bond lengths (or angles) between themagnetic manganese ions by applying
pressure has much effect on the competing
magnetic ground states in this magnetically frustrated system. In the present
study we thus performed crystal structure
analysis under pressure to elucidate whatkind of magnetic interactions between
manganese ions is essential for stabilizing
the pressure induced magnetic phase.
Crystal structure analysis was carriedout at FONDER. Hydrostatic pressure wasapplied up to p = 1.39 GPa, at which themagnetic structure is almost commensurate. Temperature was ﬁxed at T = 8 K.
Crystal structure was well solved with
R = 0.035. Figure 1 shows two different
bond lengths between Mn4+ and Mn4+
ions linked by oxygens as function of ionicradii of rare-earth ion. The interatomic
bonds shown in Fig. 1(a) and in Fig. 1(b)contribute to the magnetic interactions of
J1 and J2 , respectively, of which paths areschematically shown in Fig. 1(c). Thisﬁgure indicates that the length associatedwith J1 decreases with decreasing theionic radii. On the contrary, the length
associated with J2 is hardly affected by
the size of the ionic radii. Furthermore
in HoMn2 O5 , the bond length associatedwith J1 signiﬁcantly shortens with applying pressure while that associated withJ2 doesn’t change at all, indicating thatmagnetic interaction J1 highly contributes
to stabilizing the commensurate magnetic
phase.
References[1] H. Kimura et al.: JPSJ 77 (2008) 063704.
[2] C. R. Cruz et al.: PRB 76 (2007) 174106.

Fig. 1. (a), (b) Two different bond distances between
Mn4+ ions as functions of ionic radii of R3+ ions. (c)Schematics of magnetic structure and two different
Mn4+ –Mn4+ bonds.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-23

Hypothetical Phase Transitions and soft modes in A2BX4-type Dielectrics
H. Shigematsu(A) and K. Nomura(A)(A)Department of Physics, Faculty of Education, Shimane University
Rubidium selenate, Rb2SeO4, and Cesium
selenate, Cs2SeO4, belong to a family of
A2BX4-type (X = O, Cl, Br) crystals with
the Beta-K2SO4 type structure. As the temperature decrease, the crystals transformfrom a high-temperature phase I to an
orthorhombic phase II (Beta-K2SO4-type
structure) at T1. At lower temperature,
many of the A2BX4-type crystals, for example K2SeO4, Rb2ZnCl4 and Rb2ZnBr4,transform into an incommensurate phasewith the modulation wavevector along thea-axis at T2. However, the phase transition could not be found for many A2BO4type (X=O) crystals below T1, although
the calculated dispersion curves contain an
unstable Sigma-2 phonon branch whose
qualitative and quantitative features are
similar to those obtained for the prototype incommensurate crystal K2SeO4. Indeed, a softening tendency of the Sigma-2
phonon branch around 0.7a* was observedin Rb2SeO4 and Cs2SeO4. The estimatedhypothetical temperature is below -150 K.
In A2BX4-type (X = Cl, Br) crystals, further phase transitions take place at T3 andT4. Soft phonon mode which make contribution to the phase transition at T4 has
been observes around T-point (0,1/2,1/2).
In order to clarify the mechanism of lowtemperature phase transition and the hypothetical one in A2BO4-type crystals,
we have to obtain additional information
about the behavior of the low-energy optical branches around T-point in various
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 (0 x x) direction for K2SeO4. The lowfrequency mode softens slightly in thevicinity of x = 1/2 as the temperatureapproaches T2 = 131 K from above, anddoes not vanish, but hardens with further
decreasing temperature. In Rb2SeO4, thehollow was not observed around T-point.
The phonon dispersion frequency was essentially unchanged below room temperature. The inelastic neutron scattering study
on other A2BO4-type crystals is now inprogress.
Present address: Department of Physics,
Faculty of Education, Yamaguchi University

Fig. 1. Phonon dispersion curves in an extendedzone scheme on the (0 x x) for K2SeO4.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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1-1-24

Crystal and magnetic structure of multiferroic material BiFeO3 -BaTiO3
R. Kiyanagi, T. Yamazaki, Y. Sakamoto, H. Kimura, Y. Noda, and K. Ohyama
Institute of Multidisciplinary Research for Advanced Materials, Tohoku university, Institute forMaterials Research, Tohoku university
A perovskite compound BiFeO3 isknown as a multiferroic material withferroelectricity (TC ∼ 1100 K) and antiferromagnetism (TN ∼ 650 K). In the course of
exploration of an enhanced multiferroicityof BiFeO3 , solid solutions of BiFeO3 andother perovskite compounds have been
investigated. It has been reported thatthe solid solution of BiFeO3 and BaTiO3 ,(1-x)BiFeO3 -xBaTiO3 , exhibits weak ferromagnetism as well as the ferroelectricity inthe range of 0 ≤ x ≤ 0.5 [1]. Meanwhile,
structural studies by X-ray powder diffraction suggested that the crystal structureof (1-x)BiFeO3 -xBaTiO3 is hexagonal inx ≤ 0.33 and cubic in 0.33 ≤ x ≤ 0.92
[2]. These results are contradictory sinceneither ferromagnetism nor ferroelectricity can be realized in a cubic system.
In oder to clarify the structure of (1x)BiFeO3 -xBaTiO3 , (1-x)BiFeO3 -xBaTiO3
with various x were studied by means ofneutron powder diffraction.
The samples were synthesized by solidstate reaction from powders of Bi2 O3 ,Fe2 O3 and BaTiO3 with various molar ratios, corresponding to x = 0, 0.1, 0.2, 0.25,
0.33, 0.4, 0.45, 0.5, 0.6, 0.7, 0.8, 1.0. The neutron powder diffraction experiments werecarried out on the neutron powder diffractometer, HERMES, installed at T1-3 beam
port in JRR-3M. Each sample was measured at several temperatures between 13
K and 650 K. The obtained powder diffraction patterns were analyzed by the Rietveld
method with the General Structure Analysis System (GSAS) with EXPGUI [3, 4].
With the results of the structural analyses
on various compositions and temperatures,the phase diagram of (1-x)BiFeO3 -xBaTiO3
with respect to x and temperature was obtained as shown in Fig. 1. Coexistence ofthe hexagonal phase and the cubic phasein a wide range of x was observed. The
hexagonal phase persists up to x = 0.8, andthe cubic phase was recognized in 0.2 ≤x ≤ 0.6 at room temperature. This coexisting hexagonal phase is considered to be theorigin of the observed ferroelectricity in (1x)BiFeO3 -xBaTiO3 . Note that the hexagonal phase is rich in Bi and Fe, and the cubic
phase is rich in Ba and Ti. TN and TS , the expected structural phase transition temperature, were estimated from the magnetic reﬂection, (1 0 1), and the hexagonal-phasespeciﬁc reﬂection, (2 1 5̄), respectively. Decreases of TN and TS were found as x increased. These changes are apparently attributed to internal structural deformation,
namely the decrease of hexagonality in the
hexagonal phase surrounded by the cubic
phase.
References[1] T. Ozaki, et al.: Ferroelectrics (2009) inpress.
[2] M. M. Kumar, A. Shrinivas, S. V. Suryanarayana: J. Appl. Phys. 87 (2000)855.
[3] A. C. Larson, R. B. von Dreel: Los
Alamos National Laboratory Report LAUR
(2004)86-748.
[4] B. H. Toby: J. Appl. Crystallogr. 34(2001)210.

Fig. 1. Obtained phase diagram of (1-x)BiFeO3 xBaTiO3 with respect to x and temperature

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-25Phase transition in a lead-based inorganic-organic perovskites C5H10NH2PbI3
Miwako Takahashi(A), Munehiko Nakatsuma(A), Kunimitsu Kataoka(A), Takurou
Kawasaki(A), Ken-ichi Ohshima(A), Yukio Noda(B)(A)IMS., Univ. of Tsukuba, (B)IMRAM, Tohoku Univ.
C5H10NH2PbI3 has a lead-based
inorganic-organic perovskites structure
consisting of semiconducting parts which
are composed of one-dimensional chainsof face-sharing lead-iodide octahedra andbarrier parts composed of C5H10NH2+
molecules. The lead-iodide chain is isolated by the organic molecules to be aquantum wire, so this material can be
regarded as a naturally self-organized
one-dimensional system. The crystal structure at room temperature is orthorhombic
with space group of C2221. It has beenshown by Raman scattering, DSC andoptical absorption measurements that thestructure undergoes temperature-induced
successive phase transitions: phase I atroom temperature, phase II for 255.5K
to 284.5K, phase III for 250K to 255.5K
and phase IV below 250K, which involve
rotational/orientational ordering of theorganic C5H10NH2+ parts. However, its
precise structure has not been determinedyet. We have been studying structures andphase transitions in this material by combining the data obtained by neutron andx-ray diffraction techniques, and foundinteresting structural changes take place inthe successive phase transitions. The lattice
parameters show step-like changes at thetransition temperatures with considerable
large contraction along direction vertical tolead-iodide chain while it expands along
the chain. Below 285K in phase II, 400
peak is found to separates in two indicating that the crystal lattice changes fromorthorhombic to monoclinic. The angle
between the splitting peaks increases linearly with decreasing temperature down
to 255K and decreasing again up to room
temperature without any hysteresis. Below
255K, diffuse peaks appear at the reciprocal points at which reﬂection is forbiddenin the C-centered lattice. These results
show that the large structural changes areaccompanied with the successive phasetransitions. Structural analysis measurement for the phase II has been performedby using a single crystal diffractometer
T2-2, FONDER. Since creation of twined
crystals in the process of phase transitions
is inevitable, Bragg peak intensities were
measured at 280K just below the transition
temperature where monoclinic angle isclose to 90 degree and intensities fromtwined crystals were integrated together.
The intensity data at phase II has been
analyzed with the model of monoclinic
P21/n which has been suggested by X-ray
measurement. The reﬁnement was not successful and structure at phase I gives better
R value. Powder diffraction measurement
was also performed by using HERMES.
The obtained data shows quite high background due to the incoherent scatteringfrom H atoms. Figure 1 shows diffraction
pattern at room temperature analyzed by
the Rietveld method ”RIETAN-2000” [1].
The Rietveld analysis for the data at low
temperatures is now going on.
[1] F. Izumi and T. Ikeda, Mater. Sci. Forum,
321-324 (2000) 198-203.

Fig. 1. Diffraction pattern at phase I analyzed by
Rietveld method.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 794- 48 -

JAEA-Review 2013-039

1-1-26

Magnetic Fluctuations in a Ternary Alloy CuFePt6
M. Takahashi(A), T. Shishido(A), K. Ohshima(A), M. Matsuura(B)(A)IMS., Univ. of Tsukuba, (B)ESS., Ohsaka Univ.
without magnetic ﬁeld below Tc2. Withoutmagnetic ﬁeld, inelastic peaks have been
observed at k=0.45 and 0.65. When applying ﬁeld of only 70 Oe, peaks disappear
and intensities of higher back ground wereobserved. The results show that there exists dynamical ﬂuctuation in the magnetic
structure which is easily suppressed byweak magnetic ﬁeld. Further experiments
should be necessary to clarify the origin of
the magnetic ﬂuctuation.
[1]M. Takahashi, E. Ahmed, A. K. Das, Y.
Fujii, H. Iwasaki, and K. Ohshima; Journal of Alloys and Compounds 453, 75-78(2008).
(a)Intensity/M15000(~10sec)

2500( 0 -0.5 -0.5) at 10K
Anti-ferromagnetic peak
5G B-PG-SP-80-S-PG-80-80
Ef=14.7meV
Hex= 0 Oe
Hex=70Oe

2000
1500
1000
500
0
-0.53

-0.52

-0.51

-0.50

-0.49

-0.48

-0.47

(0,K,K) (r.l.u.)(b)Intensity/M2000K(~700sec)

CuFePt6 has fcc fundamental structureand forms Cu3Au-type ordered structure
below 1313 K[1]. In the ordered structure,
Cu and Fe occupy corner sites with equal
occupation probabilities while Pt occupies
face centered sites. In spite of the simple
atomic arrangement in the ordered structure, its magnetic behavior is complicated.
In the process of zero-ﬁled cooling (ZFC)
it undergoes successive transitions of ferromagnetic at Tc1=200K and ferrimangetic at
Tc2=100K. In the process of ﬁeld cooling, on
the other hand, only a ferromagnetic phaseappears below Tc. The behaviors indicate
existence of competitive interactions of ferromagnetic and antiferromagnetic which
are sensitively dependent on the magnetic
ﬁeld. To investigate ﬁeld dependence ofthe magnetic structure, elastic and inelastic neutron scattering measurements were
performed at the triple-axis-spectrometer
PONTA. In the measurements, intensityof magnetic scattering at around Gamma
and M points of the ordered structure havebeen investigated under FC and ZFC processes. Magnetic ﬁeld was applied up to
70 Oe with using Helmholtz coil. In order
to compare the behavior of elastic and inelastic components of magnetic scattering,elastic intensities have been measured under triple axis mode.
Figure 1(a) shows X point magnetic Bragg
scattering for FC and ZFC process. Intensities of the ferrimagnetic component does
not change under FC and ZFC processes,
though ferrimagnetic phase does not appear in the magnetization measurement. It
has been conﬁrmed in the measurements
at FONDER that ferrimagnetic component
remains under the magnetic ﬁeld of up to
1.5kOe. Ferromagnetic Bragg scattering at
Gamma point also shows no dependence ofmagnetic ﬁeld. Figure 1(b) shows inelastic
intensities of dE=2 meV along 0kk with and

200
T=10K
Hex=70 Oe

150

Hex= 0 Oe

100

50

0

-1.2

-1.0

-0.8

-0.6

-0.4

(0,k,k) (r.l.u.)

Fig. 1. (a)Magnetic Bragg scattering at X point under FC and ZFC processes. (b)Inelastic intensities
around X point with and without magnetic ﬁeld below Tc2.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 795- 49 -

JAEA-Review 2013-039

1-1-27

Kinetics of crystalline-noncrystalline phase transition of sucrose crystal
M. Takahashi(A), K. Kawasaki(A) and K. Ohshima(A)(A)Institute of Materials Science, University of Tsukuba
Sugar, in which sucrose (C12H22O11) is
the main ingredients, attracts a great dealof attention in the ﬁeld of food, medicines,
preservative and battery material adjusting
to surroundings. However, melting points
among sucrose crystals with high purity
are occasionally different from each otherand are given as in the range from 433 to459K. It has been thought that the impurity, the water content or the manufacturing method would contribute such different melting points. There are few diffraction studies for understanding of the melting phenomena, though the macroscopic
observation has been carried out by an
optical microscope and a calorimeter. We
have, therefore, performed in-situ diffraction study for the kinetics of crystallinenoncrystalline phase transition in sucrose.
Since information on the hydrogen atom
positions is indispensable, neutron diffraction measurement was performed by using a single crystal diffractometer T2-2,
FONDER. In the diffraction measurement,a sucrose single crystal with a volumeof 24mm3 was mounted in a aluminium
cell with a heater coil. Intensities of Bragg
peaks were measured at room temperature
for a structural analysis, and then the sample was heated to 366 K which is far below
the melting points. Time dependence of the
Bragg peak intensities was measured withkeeping the sample at the ﬁxed temperature.
Crystal structure at room temperature isdetermined by combination of X-ray andneutron data. Figure 1(a) shows nuclear
density distribution on a-c plane calculated by MEM using PRIMA[1]. It clearlyshows negative peaks (blue part) whichindicate hydrogen atom positions. Figure1(b) shows temperature dependence of 401
and 442 Bragg peaks. The Bragg intensities decrease monotonically indicating thatthe sample gradually changed to noncrystalline state. In the x-ray measurements,
the incubation time, which was deﬁned as
waiting time until the noncrystalline phasetransition starts at a ﬁxed temperature, hasbeen observed in a range between 422K
and 443K[2]. Time dependence of the Bragg
intensities in the present neutron measurement did not show any incubation time.
Structure analysis for the data in the successive time spans is now going on to study
microscopic change of crystalline to noncrystalline phase.
[1]F. Izumi and R. A. Dilanian, ”Recent
Research Developments in Physics,” Vol.
3, Part II, Transworld Research Network,
Trivandrum (2002), pp. 699-726.
[2]T. Fujita, Doctor Thesis of Univ. of
Tsukuba (2006).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 796- 50 -

JAEA-Review 2013-039

1-1-28

Crystal structure of Pb-free silver niobate perovskite
Masatomo Yashima, †,* Takahiro Wakita, † Takafumi Komatsu, † Yong Phat, †Hiroki Taniguchi, ‡ Tomoyasu Taniyama, ‡ and Mitsuru Itoh ‡† Department of Materials Science and Engineering, Interdisciplinary Graduate School of
Science and Engineering, Tokyo Institute of Technology, Nagatsuta-cho 4259, Midori-Ku,
Yokohama, Kanagawa 226-8502, Japan, ‡ Materials and Structures Laboratory, Tokyo Instituteof Technology, 4259 Nagatsuta-cho, Yokohama 226-8503, Japan
Lead-free piezoelectrics with high performance are important in material sciences.
Materials with a large internal polarizationthat can be strongly coupled to an electricﬁeld are required. But, the crystal structureof AgNbO3 has not been studied satisfactorily [１]. In the present work, we haveinvestigated the crystal structure and phasetransition of AgNbO3 with neutron powder diffractometry.
AgNbO3 materials were prepared by solidstate reactions. Appropriate amounts ofhigh purity Ag2O and Nb2O5 were mixed
with ethanol in an agate pot and calcinedat 980 °C for 6 h in O2 atmosphere. The
calcined powder was then milled again,pressed in a 10 mm steel die with a pressure of 1000 kgf/cm2 to make pellets, followed by sintering at 1050 °C for 6 h in
O2 atmosphere. A phase purity of AgNbO3
was conﬁrmed by x-ray diffraction measurements.
We performed neutron powder diffraction experiments on the Kinken powder
diffractometer for high-efﬁciency and highresolution measurements, HERMES [2], of
Institute of Materials Research, Tohoku
University, installed at the Japan research
reactor, JRR-3M in Japan Atomic Energy
Association, Tokai, Japan. Incident neutrons with a ﬁxed wavelength of 1.82646
were obtained by a vertically focusing (331)
Ge monochromator and a 12 -∞-22 collimator. Diffraction data were collected atstep intervals of 0.1? over a 2? range from
20 to 152?, using 150 3He counters set atintervals. We have utilized a furnace1with MoSi2 heaters [3], which was devisedfor neutron diffraction study by the HERMES, to heat the AgNbO3 rod in air un-

der atmospheric pressure at high temperatures. There were two thermocouples in the
furnace. One thermocouple near the heater
was used to control the temperature andthe other near the rod sample monitored
the sample temperature.
Figure 1 shows the Rietveld pattern of
AgNbO3 at room temperature. The reliability factors were Rwp=5.41%, RB=1.96%
and RF=0.98%. Unit-cell parameters, b=5.6091(3)andwere a=5.5526(3). Increasing temperaturec=15.6462(7)phase transitions were observed.
References
1.
D. Fu, M. Endo, H. Taniguchi, T.
Taniyama and M. Itoh, Appl. Phys. Lett.,
90, (2007) 252907.
2. K. Ohoyama, T. Kanouchi, K. Nemoto,
M. Ohashi, T. Kajitani and Y. Yamaguchi, Y.
Jpn. J. Appl. Phys. Part 1, 37 (1998) 3319.
3. M. Yashima, J. Am. Ceram. Soc., 85 (2002)
2925.

Fig. 1.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 819- 51 -

JAEA-Review 2013-039

1-1-29Structure Analysis of Oxide Ions in a Doped Pr2NiO4-based Mixed Conductor
Hiroki Yamada † , Masatomo Yashima † , Tomoya Takizawa † , Shinji Yamamoto † ,Tatsumi Ishihara ‡† Department of Materials Science and Engineering, Interdisciplinary Graduate School of
Science and Engineering, Tokyo Institute of Technology, Nagatsuta-cho 4259, Midori-ku,
Yokohama, Kanagawa 226-8502, Japan and ‡ Department of Applied Chemistry, Faculty ofEngineering, Kyushu University, Motooka 744, Nishi-ku, Fukuoka 819-0395, Japan
Mixed oxide-ionic and electronic conducting ceramics (MIECs) are attracting muchinterest as materials for oxygen separation membranes. Oxygen can permeate
through MIECs membranes when a gradient of oxygen chemical potential exists. A2BO4-based oxides with K2NiF4type structure have extensively been studied as a new mixed ionic-electronic conductor, where A and B are cations. The
development of improved MIECs requires
a better understanding of the mechanismof ionic conduction, and crucial to thisis a comprehensive knowledge of the oxide ion conduction in the A2BO4-basedoxides occurs by diffusion of excess oxide ions along the rock-salt-type AO layers. However, the diffusion of excess oxide ion has not been determined yet.
Pr2NiO4-based oxides have high oxygen
permeability and high diffusivity of oxide ions. Here, we report the structure
analysis of a K2NiF4-type mixed conductor Pr2(Ni0.75Cu0.25)0.95Ga0.05O4+δ
(PNCG), through a high-temperature neutron powder diffraction study. We chose
this chemical composition, because it
exhibits high oxygen permeability. The
present result would give hints for the design of K2NiF4-type conductors.
A PNCG sample was prepared by a solidstate reaction at 1350 oC for 6 h in air. Neutron powder diffraction data of PNCG werein situ measured at 20.4-1011.2 oC using
a furnace and 150 detector system HERMES at a neutron wavelength of 1.8204(5)angstrom. Neutron diffraction data wereanalyzed by Rietveld analysis. A computer
program RIETAN-FP was utilized for the
Rietveld analysis.

Rietveld reﬁnements of the neutron diffraction data of PNCG at 20.4 oC and 1011.2 oC
were performed on the basis of the K2NiF4type structure with I4/mmm space-groupsymmetry. Reliability factors and goodnessof ﬁt at 20.4 oC were Rwp = 6.66%, RI =3.06%, RF = 1.78% and GOF = 3.17. Lattice parameters were a = b = 3.8364(2)angstrom, c= 12.5374(7) angstrom. Reliability factors and goodness of ﬁt at 1011.2
oC were Rwp = 6.33%, RI = 2.06%, RF =0.98% and GOF = 4.93 (Fig.1). Lattice parameters were a = b = 3.8793(4) angstrom,c= 12.7326(13) angstrom.

Fig. 1. Neutron diffraction proﬁles at 1011.2 oC
for Pr2(Cu0.75Ni0.25)0.95Ga0.05O4+δ using a single phase I4/mmm model.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 824- 52 -

JAEA-Review 2013-039

1-1-30

Structure analysis of automotive exhaust catalysts, Ce2Zr2O7.32 by neutron
powder diﬀraction measurement
Tomoya Takizawa, Masatomo Yashima, Takahiro Wakita
Department of Materials Science and Engineering, Interdisciplinary Graduate School of Scienceand Engineering, Tokyo Institute of Technology, Nagatsuta-cho 4259, Midori-Ku, Yokohama,
Kanagawa 226-8502, Japan
CeO2-ZrO2 solid solutions have been investigated due to their high oxygen storage capacity [1,2]. In particular, it is known
that Ce2Zr2O7+x (0<x<1) has higher oxygen storage capacity in CexZr1-xO2-d solid
solutions. Sasaki et al reported Ce2Zr2O7
and Ce2Zr2O7.5 belong to the Fd-3m andF-43m space groups, respectively [3]. However, structure analysis of Ce2Zr2O7+x(0<x<1) has not been studied satisfactorily. In this study, we report the structure
analysis of Ce2Zr2O7.32.
Ce2Zr2O7 powders were prepared by a coprecipitation route. The amount of oxygen
atom was analyzed by thermogravimetricmeasurement, and the composition of sample was determined as Ce2Zr2O7.32. The
powders were put into vanadium holder
and neutron powder diffraction measurement was performed in air with a 150detector system, HERMES [4], installed at
the JRR-3M reactor in Japan Atomic Energy
Agency, Tokai, Japan. Neutron with wavelength 1.81386 angstrom was obtained bythe (331) reﬂection of a Ge monochromator. Diffraction data were collected in air at
299.7 K. The experimental data were analyzed by Rietveld method. Computer program RIETAN-FP [5] was utilized for the
Rietveld analysis.
Rietveld analysis of Ce2Zr2O7.32 at 299.7
K was carried out assuming the F-43m
space group. The reliability factors andgoodness of ﬁt were Rwp = 8.64%, RI =1.63%, RF = 0.85% and S = 3.70. Unitcell parameter was 10.6404(3) angstrom.
Atomic displacement parameters of cation
and anion were 0.0043(5) and 0.0097(5)angstromˆ2, respectively.

[1] M. Yashima et al., J. Am. Ceram. Soc. 76(1996) 2865.
[2] M. Yashima et al., Appl. Phys. Lett. 72(1998) 182.
[3] T. Sasaki et al., J. Ceram. Soc. Japan. 112(2004) 440[4] K. Ohoyama et al., Jpn. J. Appl. Phys. 37(1998) 3319.
[5] F. Izumi and K. Momma, Solid State
Phenomena. 15-20 (2007) 130.

References
Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 825- 53 -

JAEA-Review 2013-039

1-1-31

Lattice dynamics of cubic NaNbO3
I. Tomeno(A), Y. Tsunoda(B), K. Oka(C), M. Matsuura(D), M.Nishi(E)(A)Akita Univ., (B)Waseda Univ., (C)AIST, (D)Osaka Univ., (E) Univ. of Tokyo

25

Energy (meV)

20

TO Σ3

15

10

TA Σ3

5

M3
0
0.0

0.1

0.2

0.3

0.4

0.5

0.4

0.5

[ζζ0]
25

20

15
E (meV)

Sodium niobate NaNbO3 has a simple
cubic perovskite structure above Tc1 =913
K. NaNbO3 undergoes at least six phasetransitions. First, the cubic to a tetragonal phase transition takes place at Tc1 .
Next, three distinct orthorhombic phases
appear between Tc5 =643 K and Tc2 =848 K.
An AF monoclinic P phase exists in therange between Tc6 =193 K and Tc5 . Finally, NaNbO3 exhibits a FE rhombohedral N phase below Tc6 . We studied
the phonon dispersion relations for cubic
NaNbO3 . The inelastic-neutron-scatteringexperiments were mainly performed using
the T1-1 triple-axis spectrometer. Most of
the measurements were performed at 970
K.
The important features of the phonon
dispersion are the simultaneous softeningof M3 and R25 phonon modes. Present results indicate the instabilities of in-phaseand out-of-phase rotations of the oxygen octahedra about the [001] direction.
These zone-boundary modes exhibit an extremely gradual softening as the temperature is lowered toward Tc1 =913 K. Figure
1 shows the phonon dispersion relations
along the [110] direction. The TO1 phononmodes along the [110] direction polarizedwith the [001] direction also soften aroundq=[0.15,0.15,0] and merge into the lowerenergy TA phonon modes. This is basically similar to the waterfall phenomenon
observed for Pb-based perovskite relaxor
ferroelectrics. The coexistence of longwavelength and zone-boundary phonon
instabilities above Tc1 =913 K is closely related to the complex sequence of phasetransitions in NaNbO3 .

TO Σ4
10

TA Σ4

5

0
0.0

0.1

0.2

0.3

[ζζ0]

Fig. 1.
Phonon dispersion relations for cubic
NaNbO3 at 970K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 841- 54 -

JAEA-Review 2013-039

1-1-32

Phonons in tetragonal BiVO4
I. Tomeno(A), N. Sato(A), K. Oka(B)(A)Akita Univ., (B) AIST
that the TA phonon branch at T=533 K havea relatively ﬂat slope in the vicinity of zone
center. We also found a central peak associated with the softening of TA modes.
Further experiments are necessary to investigate the lattice dynamics of tetragonal
BiVO4 in a wide temperature range.
References [1]G. Benyuan, M. Copic and
H. Z. Commins, Phys. Rev. B24, 4098
(1981). [2]H. Tokumoto and H. Unoki,Phys. Rev. B27, 3748 (1983).
BiVO4

6
q=[
5

ξcosθ,E (meV)ξsinθ, 0 ]θ = 45°4

θ = 35°3

T = 533 K

2
1
0
0.0

(a)
0.1

0.2

0.3

0.4

0.5

ξ (r.l.u.)
6
5

q=[

ξcosθ,

ξsinθ, 0 ]θ = 35°4
E (meV)

Bismuth vanadate BiVO4 undergoes asecond-order ferroelastic phase transition
at TC =525 K. The high-temperature paraelastic phase has a tetragonal scheelite struc6 ).
Inture with space group I41 /a (C4hthe sheelite structure, the isolated VO4tetrahedra are separated by the Bi3+ ions.
The low-temperature ferroelastic phase has
a monoclinic distorted scheelite structure
6 ). Brillouin scattering studies
with I2/a (C2hrevealed a dramatic softening of transverse
acoustic (TA) modes polarized on the (001)plane at TC .[1-2] We studied the lattice dynamics of BiVO4 in the paraelastic phase.
Inelastic neutron scattering measurements
were performed using the triple-axis spectrometer T-11 (HQR) at JRR-3M.
We performed
transverse
constant-Q√√
scans at q = [ 2ξ cos θ, 2ξ sin θ, 0] polarized in the (001) plane, where θ is an absolute value of the angle from [100] in the(001) plane. The angular dependence of
the TA phonon energy corresponds reasonably to the results of Brillouin-scatteringstudies. Figure 1 shows that a difference in the√ energy ◦between√ TA phonon
2ξ sin 35 , 0] andq = [ 2ξ cos 35◦ ,q = [ξ, ξ, 0] becomes large with increasing ξ. These results demonstrate thatthe acoustic symmetry axes in a tetragonal scheelite structure deviate from thecrystallographic high-symmetry [ξ, ξ, 0] direction. We measured the phonon
dis√
◦,
[
2ξ
cos
35
persionrelation
along
the
√
2ξ sin 35◦ , 0] direction at T=533 and 773
K. The results plotted in Fig.1(b) indicate that√ of the◦ TA mode
√ the softening2ξ sin 35 , 0] occurs
along [ 2ξ cos 35◦ ,in the small ξ region. Brillouin-scattering
measurements revealed that the frequencyofpropagating along the√√ the TA phonon[ 2ξ cos 35◦ , 2ξ sin 35◦ , 0] direction becomes small toward Tc . Thus we expect

773 K
533 K

3
2
1
0
0.0

(b)
0.1

0.2

0.3

0.4

0.5

ξ (r. l. u. )Fig. 1. The TA phonon dispersion curves in tetragonal BiVO4 .

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 842- 55 -

JAEA-Review 2013-039

1-1-33Inelastic neutron scattering in the impurity-induced ferroelectric phase of
CuFe1−y Gay O2
N. Terada1 , T. Nakajima2 , and S. Mitsuda2
1 National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, 305-0047
2 Fac. of Sciences, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo, 162-0825
Since the discovery of the magnetic-ﬁeldinduced ferroelectric phase transition in
CuFeO2 ,[1] the magnetoelectric couplingin this compound has attracted considerable attention. Although the static features,such as magnetic structure and ferroelectric
polarization, in this system have been relatively well understood, the magnetic excitation has not been fully understood so far.
This time, in order to determine thespin wave dispersion relation of thenonmagnetic impurity induced ferroelectric incommensurate (FEIC) phase in
CuFe1−y Gay O2 , we have performed the inelastic neutron scattering measurements on
CuFe0.965 Ga0.035 O2 . Unlike the FEIC phaseof the Al-doped sample with spatiallydistributed magnetic domains with two
different wave numbers, the FEIC phase of
the Ga-doped sample is characterized by asingle wave number.[2]The experiment was carried out with thecold neutron triple-axis spectrometer HER
installed at C1-1 beam port in the guide hallof JRR-3. The single crystal sample is of themass 4.8 g. Constant E f (= 3 meV) mode
was used. To cut off the higher order contamination, the Be ﬁlter was put back of thesample.
As shown in Fig.
1, we obtained
the contour map of the neutron scattering intensity corresponding to the dynamic structure factor S(Q, ω ) along the[H, H, 3/2] direction in the FEIC phaseof CuFe0.965 Ga0.035 O2 . In the previous
neutron diffraction measurements[2], theBragg reﬂections at (q q 32 ) and ( 12 − q 12 −q 32 ) with q = 0.203 were observed. The
lowest energy spin wave branch starts fromthe two reﬂection points, where the energy
gap of the branch is smaller than 0.2 meV.

We conﬁrmed that the spin wave with energy gap in the 4-sublattice (4SL) phase ofpure system of CuFeO2 [3, 4] is soften andthe energy gap goes to zero by a small
amount of nonmagnetic impurity.
The relatively complex dispersion relation has not been solved completely at thepresent stage. There are two types of modelfor geometric pattern of the exchange interaction. One is a simple triangular latticemodel that is considered up to third nearest neighbor exchange interactions, which
was applied to the pure CuFeO2 by theother group.[4] However, the lattice distortion occurs in both the 4SL and the FEIC
phases. We therefore expect that the scalene triangular lattice model, where thenearest neighbor interactions splits into thethree different interactions as the result of
the lattice distortion, could explain the dispersion relation.
References[1] T. Kimura et al.: PRB 73, 220401 (2006).
[2] N. Terada et al.: PRB 78 014101 (2008).
[3] N. Terada et al.: JPCM 19 145241 (2007).
[4] F. Ye et al.: PRL 99 157201 (2007).

Fig. 1. The spin wave dispersion relation along the[H, H, 3/2] direction in the ferroelectric incommensurate phase of CuFe0.965 Ga0.035 O2 .

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 846- 56 -

JAEA-Review 2013-039

1-1-34

Crystal structure analyses of layered thermoelectric manganites
Yuzuru Miyazaki, Fumiya Kawashima, Kei Hayashi and Tsuyoshi Kajitani
Department of Applied Physics, Graduate School of Engineering, Tohoku University
Perovskite based layered manganites haverecently attracted much interest owing totheir high n-type thermoelectric (TE) performance at higher temperatures. We havestudied the effects of detailed structure, inparticular the Mn-O distances and Mn-OMn angles, on the TE properties. Here,
we report the structure of Sr- and (Bi, Sr)substituted Ca2MnO4 at room temperature; the chemical formulas of the substituted samples are (Ca1.4Sr0.5Bi0.1)MnO4
and (Ca1.5Sr0.5)MnO4. Neutron powder
diffraction (ND) data were collected at several temperatures by the use of HERMES
diffractometer. The ND data were analyzed using the Rietveld reﬁnement program RIETAN2000. In Fig.1(a), we show
the observed, calculated and difference
patterns of ND data for Ca2MnO4, basedon the I41/acd space group. All the samples were reﬁned with the identical spacegroup and converged with reasonably low
R-factors. In Fig.1(b), we plot the relationship between the effective ionic radii (Reff)at the Ca site and the Mn-O2 distance aswell as the Mn-O2-Mn angles of the MnO6octahedra. With increasing Reff, both thedMn-O lengths and Mn-O2-Mn angles increase. The increase in the Mn-O2 lengths
reduces the overlapping of the Mn3d-O2p
orbitals, while the increase in the Mn-O2Mn angles enhances such overlapping. In
fact, the latter effect plays a dominant role
to increase TE performance and a further
substitution by Sr would be effective to prepare potential n-type TE materials in the
Mn-oxides.

Fig. 1. Rietveld reﬁnement patterns of Ca2MnO4(a) and the relationship between the effective ionicradii (Reff) at the Ca site and the Mn-O2 distances
as well as the Mn-O2-Mn angles of the MnO6 octahedra (b).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-35

Low-Energy Phonon Anomaly of CeRu4 Sb12
K. Iwasa1 , R. Igarashi1 , L. Hao2 , Y. Murakami1
Tohoku Univ.1 , China Institute of Atomic Energy2
property among the rare-earth ﬁlled skutterudite with the Sb cage.
500
CeRu4Sb12
Q = (6 -0.4 -0.4)
400Counts / 4000 MN (360 sec)

300 K

300

250 K
200 K

200
150 K
100 K
100
50 K

0

13 K
0

2

4

6

8

10

Energy [meV]

4.4
Peak position [meV]

Anomalously anharmonic lattice properties of the rare-earth ﬁlled skutterudites
RT4 X12 (R = rare earth, T = transition metal,
X = pnictogen) have been studied, in addition to the various strongly correlated electron phenomena originating from 4 f electrons. The ﬁlled ions locating within the
icosahedral X cage vibrate with large amplitude, as evidenced by the large DebyeWaller factors. One of the attractive lattice properties is the dispersion of elastic
constants of PrOs4 Sb12 , interpreted as lowenergy Pr-ion motion within the Sb cage (T.
Goto et al.: Phys. Rev. B 69 (2004) 180511).
We have reported the anomalous softening of phonon due to Pr vibration withdecrease of temperature and 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 the present
study, we have investigated the low-energy
phonon spectra of CeRu4 Sb12 using thetriple-axis spectrometer TOPAN (6G).
The ﬁgure shows temperature dependence of the peak energy position corresponding to the phonon excitation measured at the reciprocal lattice point Q =(6 -0.4 -0.4) of CeRu4 Sb12 . It shows decreasing behavior of excitation energy withdecreasing temperature from 300 down to
13 K. This softening mode was conﬁrmed
to be less dispersive like an optical mode
assigned to the Ce motion in the Sb cageof CeRu4 Sb12 (C. H. Lee et al.: J. Phys.
Soc. Jpn. 75 (2006) 123602). The presenceof such anharmonic low-energy phononis seen also in the previously investigatedthree compounds of PrOs4 Sb12 , PrRu4 Sb12 ,CeOs4 Sb12 which was reported in the Meeting of Physical Society of Japan (Sep. 2007).
Therefore, the anharmonicity appearng in
the low-lying optical mode of rare earth
ions inside the Sb cages is a characteristic

4.3

CeRu4Sb12
Q = (6 -0.4 -0.4)

4.2
4.1
4.0
3.9
0

50

100 150 200 250 300
Temperature [K]Fig. 1. Temperature dependence of the phonon
spectra and the peak energy at Q = (6 -0.4 -0.4) ofCeRu4 Sb12 .

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-36

Neutron Diﬀraction Study on SnO2-MOx (M = Ce, Sb) System
K. Nomura (A), H. Kageyama (A), T. Maekawa (B), C. Minagoshi (B), H. Miyazaki (B),and Y. Kawabata (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 a previous study, wemeasured the neutron diffraction data of
SnO2-MOx (M = Al, Ce) system [2], and investigated the crystal structure and the nuclear density distributions. In this study,
we have investigated the crystal structure
and the nuclear density distributions of
SnO2-MOx (M = Ce, Sb) system.
Neutron diffraction measurements ofhighpurity(SnO2)(CeO2)a(SbOx)b(0.01<=a<=0.03, 0.01<=b<=0.03) samples
were performed with HERMES installedat JRR-3M in JAEA (Tokai) [3]. Neutron
wavelength was 1.8204(5)A. Diffraction
data were collected in the 2 θ range
from 20 to 157 deg. in the step intervalof 0.1 deg.
The diffraction data obtained were analyzed by the combination
technique of Rietveld analysis using acomputer program RIETAN-2000 [4] and amaximum-entropy method (MEM)-based
pattern ﬁtting. MEM calculation was
carried out using a computer program
PRIMA [5].
The neutron diffraction patterns of(SnO2)(CeO2)a(SbOx)b (0.01<=a<=0.03,
0.01<=b<=0.03) samples showed larger
peak widths and higher background intensities compared to that of pure SnO2.
All the reﬂection peaks of these samples
were indexed by a tetragonal symmetry(P42/mnm, No.136). The assumed structure model was as follows: Sn, Ce, andSb atoms occupy 2a sites (0, 0, 0) and O

atoms occupy 4f sites (x, y, 0) (x = y ˜ 0.306)[1] with isotropic atomic displacement
parameters. The lattice parameters andunit cell volume increased with increasing
Ce and (or) Sb contents, suggesting the
introduction of larger Ce4+(0.97A) and(or) Sb3+(0.76A) ions [6] into Sn4+ (0.69A)
sites. Figure. 1 shows the equicontour surfaces (0.5fm/Aˆ3) of scattering amplitudeof (SnO2)(CeO2)0.03(SbOx)0.03. Not only
2a (Sn, Ce, Sb) sites but also 4f (O) sites
showed nonspherical equicontour surfaces
with large distributions (compared toSnO2), suggesting the disturbed atomic
arrangements on the 2a and 4f sites byintroducing Ce and Sb atoms into Sn sites.
References[1] M. Batzill and U. Diebold, Progress in
Surface Science, 79, 47 (2005).
[2] T. Maekawa, C. Minagoshi, S. Nakamura, K. Nomura, H. Kageyama, Chemical
Sensors, 24, 19 (2008).
[3] K. Ohoyama, T. Kanouchi, K. Nemoto,
M. Ohashi, T. Kajitani, and Y. Yamaguchi,
Jpn. J. Appl. Phys., 37, 3319 (1998).
[4] F. Izumi and T. Ikeda, Mater. Sci. Forum,
321-324, 198 (2000).
[5] F. Izumi and R.A. Dilanian, in: Recent
Research Developments in Physics, vol.3,
Transworld Research Network, Trivandrum, 2002, p.699.
[6] R.D. Shannon, Acta Cryst, B51, 751(1976).

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1-1-37

Observation of Hydrogen Tunneling in Pd nanoparticles by Low-temperature
Neutron Scattering Measurement
Miho Yamauchi(A), Hiroshi Kitagawa(B), Osamu Yamamuro(C)(A)CRC, Hokkaido Univ., (B)Faculty of Sci. Kyushu Univ., (C)ISSP-NSL Univ. Tokyo
2H NMR spin-lattice relaxation times (T1)for deuteron atoms in the Pd nanoparticles showed a particular minimum below
30 K while T1 for the bulk sample increase monotonously with decreasing temperature. In order to clarify the origins of
the unusual T1 minima, neutron scatteringexperiments were carried out for the bulk
and nanoparticle of Pd with AGNES spectrometer installed at JRR-3 (JAEA, Japan).
Pd nanoparticles, that are homogeneous in
size, were synthesized by a chemical reduction method with water-soluble polymer, poly[N-vinyl-2-pyrrolidone] abbreviated as PVP. By TEM measurements, homogeneity in size of Pd nanoparticles was
conﬁrmed and the mean diameter was estimated to be 6.3 ± 1.0 nm. 800 mg of Pd
nanoparticles were loaded into the sample tube that was connected to a vacuum line and a hydrogen gasbag. In thissystem, pressure inside the sample tube
can be monitored and hydrogen gas provided. Measurements for bulk Pd and Pd
nanoparticles with and without hydrogengas were performed at 7, 14 and 28 K.
The data were accumulated for 32 hours.
Scattering intensity from absorbed hydrogen atoms was evaluated from the intensity difference between the samples withand without hydrogen atoms. Difference
scattering intensities for the Pd nanoparticle are shown in Fig. 1. Although, in general, scattering intensity is increased dueto thermal vibration, that is, the intensity
at high temperature is larger than that at
low temperature, the scattering intensity at
7 K of hydrogen absorbed in Pd nanoparticles seems to be slightly larger than that at
28 K under magniﬁcation in the energy region below 3 meV. This unusual tendencyof the scattering intensity is attributed tothe same origin of the NMR T1 minima ob-

served below 30 K.

Fig. 1. Fig. 1. Scattering intesity of hydrogen absorbed Pd nanoparticles.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 880- 60 -

JAEA-Review 2013-039

1-1-38Structural, magnetic and thermoelectric properties of half-Heusler compounds
G. Nakamoto (A), H. Murakami (A), M. Kurisu (A), A. Tanaka (B), T. Tsutaoka (B), Y.
Andoh (C)(A) School of Materials Science, Japan Advanced Institute of Science and Technology, (B)Graduate School of Education, Hiroshima University, (C) Faculty of Regional Sciences, Tottori
University
Recently, half-Heusler compounds haveattracted much attention because of thehigh potential as a thermoelectric material originating from the anomalous electronic band structure near the Fermi level
called a half-metallic state. It has been reported ﬁrstly that the TiNiSn-based halfHeusler compounds show the high thermoelectric performance with the dimensionless ﬁgure of merit, ZT=1.5 at 700 K[1]. Our group has investigated the thermoelectric property of the rare-earth basedhalf-Heusler compounds RPdSb (R: rareearth elements). The Seebeck coefﬁcient,electrical resistivity and thermal conductivity have been measured as a functionof temperature. It is found that the temperature dependence and absolute valuesof theses thermoelectric quantities depend
strongly on the sample-preparation condition. It is also expected that defects or instability of the lattice giving strong inﬂuenceon the electronic state are easily introducedin the half-Heusler structure. However, theeffect of the structural property on the thermoelectric one has not been fully understood yet in the half-Heusler system.
In the present study, in order to elucidate the correlation between the structural and thermoelectric properties in thehalf-Heusler compounds, the powder neutron diffraction study have been performedon the rare-earth based half-Heusler RPdSb
system to examine the existence of defects
and the degree of disorder. Furthermore,
the magnetic properties like the magnetictransition temperature and magnetic moment have been also investigated.
The polycrystalline samples were prepared by arc melting the constituent elements in puriﬁed Ar atmosphere. The ex-cess amount of Sb was added to compensate the weight loss due to evaporation during melting. The ingot was melted
and ﬂipped over several times to ensure
the complete mixing of the elements. The
single-phase formation was conﬁrmed bya powder X-ray diffraction measurement.
The thermoelectric and magnetic properties were studied below room temperature by a PPMS and a SQUID magnetometer. The powder neutron diffraction experiments were carried out by the T1-3, HERMES installed at JRR-3M in JAEA. The precise structural reﬁnement of the powder
neutron diffraction data was performed by
the Rietveld analysis using the pattern proﬁle ﬁtting program, RIETAN-2000 to determine the crystal parameters.
The detailed structural analysis is now
under way to have a deﬁnite conclusion
about the correlation between the structural and thermoelectric properties in thehalf-Heusler compounds.
Reference[1] N. Shutoh and S. Sakurada, 22nd International Conference on Thermoelectrics(2003), p. 312.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 890- 61 -

JAEA-Review 2013-039

1-1-39Dependence of crystal structure and thermodynamic stability on diﬀerent
synthetic method and Li content for Lix(Ni,M)O2 (M=Mn,Co) as a cathodeactive material for Li ion battery
Yasushi Idemoto, Naoto Kitamura and Takuya Hasegawa
Department of Pure and Applied Chemistry, Faculty of Science and Technology, Tokyo
University of Science, 2641 Yamazaki, Noda-shi, Chiba 278-8510
As a cathode active material for lithium
ion battery, LiCoO2 with a layer structure is the most widely used. Due tohigh cost and high toxicity of the Co,
however, nickelate-based materials havedrawn much attention. From such background, we have studied Lix(Ni,M)O2(M=Mn,Co); especially LixMn0.5Ni0.5O2
and LixNi0.8Co0.2O2, which have lower
Co content. As a result, we found that theircathode performance depended on the synthetic process. However, less informationon their crystal structures make the synthetic process effects ambiguous at this moment.
In this work, we investigated crystal structures of LixMn0.5Ni0.5O2 andLixNi0.8Co0.2O2 prepared by two different methods. We investigated the crystal
structures by Rietveld analysis using neutron diffraction and nuclear densities by
MEM. Based on the results, we discussed
relationship between thermodynamic stability, crystal structure and cathode performance, and then tried to reveal how thesynthetic process affected them.
LixMn0.5Ni0.5O2 and LixNi0.8Co0.2O2
were prepared by two methods; that is,conventional solid-state method and solution method using citric acid as an additive. Their cathode performances werestudied by CV and charge-discharge cycle
tests. In order to clarify crystal structure at
the charged state, chemical delithiation using 0.5N-(NH4)2S2O8 was also performed.
Thermodynamic stabilities of the samples
were evaluated from their heats of dissolution which were measured by a twintype multi-calorimeter. The crystal struc-tures were determined by neutron diffraction using HERMES[1] of IMR at JRR-3M
in JAERI. The data was reﬁned using the
Rietan-FP[2]. The nuclear densities were
determined with PRIMA program[3].
From XRD patterns, it was foundthat main phases of LixMn0.5Ni0.5O2(x=0.98˜1.08) synthesized in this work had
the α-NaFeO2-type layer structure (S. G.:
R-3m) although Li2MnO3 was slightly observed as a secondary phase depending
on preparation process. Cycle performance
tests revealed that the samples with thesame analytical composition exhibited different cathode performance depending on
synthetic method, that is, the samples synthesized by solid state reaction exhibit
more stable cycle performance than those
prepared by solution method. From formation enthalpies of the samples evaluated by the calorimetry, it could be concluded that higher thermodynamic stability induced better cathode performance.
In order to discuss effects of thesynthetic processes on their crystal structure, the Rietveld analysis using the neutron diffraction was carried out. As a result, it was found that cation mixing ―that is, Ni content at Li site and Li content at Ni site ― was essentially independent of the synthetic process. However, local distortion around the transition
metal site, which was evaluated from theresults of the Rietveld analysis, was larger
in the samples exhibiting worse cycle performance. Such a distortion also became
larger by a chemical delithiation although
the crystal structure kept the layer structure even after the delithiation. In the case

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

of LixNi0.8Co0.2O2[4], similar results to
LixMn0.5Ni0.5O2 were also obtained.
[1] K. Ohoyama, T. Kanouchi, K. Nemoto,
M. Ohashi, T. Kajitani, Y. Yamaguchi, Jpn.
J. Appl. Phys. 37, 3319 (1998) .
[2] F. Izumi, and T. Ikeda, Mater. Sci. Forum, 321, 198 (2000).
[3] F. Izumi and R. A. Dilanian, Recent
Research Developments in Physics, Vol.3,
Part II, Transworld Research Network,
Trivandrum (2002), pp.699-726.
[4] Yasushi Idemoto, Yu Takanashi, Naoto
Kitamura, J. Power Sources, 189(1), 269(2009).

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1-1-40

Crystal structure and ionic conduction path of Ln2Ni1-xCuxO4+d for solid oxide
fuel cells
Yasushi Idemoto and Naoto Kitamura
Departme nt of Pure and Applied Chemistry, Faculty of Science and Technology, Tokyo
University of Science, 2641 Yamazaki, Noda-shi, Chiba 278-8510
Recently, solid oxide fuel cell (SOFC)
has drawn much attention, and many researches on the device have been carriedout. Lanthanum nickelate-based materials
with the K2NiF4-type structure are considered as promising candidates for cathodes of SOFC. It is well-known that excess oxygens are incorporated at interstitial sites in the rock-salt La2O2 layer andthe oxygens can be a conduction species
in the lanthanum nickelate-based materials. Due to the difﬁculty in an analysis on
crystal structures at elevated temperature,
however, it is still ambiguous how the host
crystal structure affects excess oxygen sites
and their conduction path.
From such background, we investigated Ln2Ni1-xCuxO4+d with the K2NiF4type structure in this work. By using neutron diffraction patterns, crystal structuresof the materials at high temperature werereﬁned with the Rietveld method, and their
nuclear density distributions were also estimated by the maximum entropy method(MEM).
We synthesized LaNi0.8Cu0.2O4+d witha solution method using citric acid as anadditive. Phase identiﬁcation of the sample
was carried out by XRD, and the composition was evaluated by ICP. Conductivity ofthe sample was also measured at elevatedtemperature. In order to study the crystal structure in detail, we measured neutron diffraction patterns at the temperature
range from 298 to 673 K using HERMES
of IMR at the JRR-3M[1], and analyzed thepatterns with the Rietan-FP[2]. We also estimated nuclear density of the sample by
MEM technique with PRIMA program[3].

tions that LaNi0.8Cu0.2O4+d had a single
phase of the K2NiF4-type structure. From
ICP measurement, it was indicated thatmetal composition of the sample was almost equal to the nominal one.
As for the lanthanum nickelate-based
sample, Rietveld analysis using neutron
diffractions was performed. In the analysis,
we assumed the space group as I4/mmm
and excess interstitial oxygens in the rocksalt layer. As a result, it was found thatlattice constants of the material increased
as temperature increased. The content of
the excess oxygen, which was calculated
from the occupancy, became lower with increasing temperature although their sites
were essentially independent of temperature. Because bond valence sum of (Ni,Cu)
site became lower at higher temperature,
it was considered that the effective negative charge of the excess oxygens was compensated by an oxidation of Ni and/or Cu.
From the nuclear density distribution at elevated temperature, it was suggested thatoxygens at the interstitial site and an apex
site of the perovskite layer moved signiﬁcantly compared with the other oxygens.
[1] K. Ohoyama, T. Kanouchi, K. Nemoto,
M. Ohashi, T. Kajitani, Y. Yamaguchi, Jpn.
J. Appl. Phys. 37, 3319 (1998) .
[2] F. Izumi, and T. Ikeda, Mater. Sci. Forum, 321, 198 (2000).
[3] F. Izumi and R. A. Dilanian, Recent
Research Developments in Physics, Vol.3,
Part II, Transworld Research Network,
Trivandrum (2002), pp.699-726.

It was conﬁrmed with X-ray diffracActivity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-41

Structural Analysis of Interface between DLC ﬁlms Having Various Wettabilities
and Lubricants Using Neutron Reﬂectometry*Tomoko Hirayama, *Takashi Torii, *Takashi Kashihara, *Takashi Matsuoka, **Kazuko
Inoue, ***Masahiro Hino
*Doshisha University, **Waseda University, ***Kyoto University
Structures of interfaces between materials
and lubricants were analyzed using neutron reﬂectometry and discussed in the series of studies. In this paper, three kindsof DLC ﬁlms having various wettabilities(normal DLC, hydrophilic DLC and hydrophobic DLC) were prepared as base materials, and water and 2-propanol were selected as lubricants. The instrument weused was a neutron reﬂectometer ’MINE’
in Japan Atomic Energy Agency (JAEA).
The DLC ﬁlms were soaked into the lubricants in a specially-designed sample
holder, and the neutron reﬂectivity proﬁlesfrom the interface between DLC ﬁlms andlubricants were directly obtained. Throughan analytical ﬁtting approach with Parratt’s
theory to the obtained proﬁles, authors presented the strict structure of the interface.
First, each DLC ﬁlm was soaked into water in a sample holder, and the neutron
reﬂectivity proﬁles from the interface between DLC ﬁlms and water were obtained.
Then, deuterated water (D2O) was used forclearer analysis because of its high sensitivity for neutron. Fitting operation to theobtained reﬂectivity proﬁles showed thatdensity of water at the interface between
normal DLC and water was same as density of bulk water and uniform along vertical direction. On the other hand, at the interface between hydrophilic DLC and water, water was inﬁltrating from the top surface of DLC to the 15 nm depth. In addition, we found that the ’dense water layer’
existed from the top surface of DLC to the
2 nm depth. At the interface between hydrophobic DLC and water, ’low density
water layer’ existed on the ﬁlm surface. The
ﬁtting approach conﬁrmed that the thickness of the layer on the hydrophobic surface was 3nm, and its density was almost

half of bulk water.
Structures of interfaces between each
DLC ﬁlm and deuterated 2-propanol(CD3CD(OD)CD3) were also analyzed
using neutron reﬂectometry. We found thatthe 2-propanol was also inﬁltrating fromthe top surface of hydrophilic DLC to the
15 nm depth and was inﬁltrating from the
top surface of normal DLC to the 9 nm
depth.
The coefﬁcients of friction of each DLC
ﬁlm under boundary lubricated condition
were measured using a ball-on-disk friction tester. The ball material and size are
SUJ2 and 3/16 inch in diameter. The applied load to the ball was 0.2 N. The obtained coefﬁcient of friction of each DLC
ﬁlm under water lubricated or 2-propanol
lubricated condition is shown in Fig. 1. Thisﬁgure shows that the friction coefﬁcient ofhydrophilic DLC is lower and that of hydrophobic DLC is higher than that of normal DLC. It may be because that for thehydrophilic surface, lubricants are enoughto reduce the friction, while that for thehydrophobic surface, friction surface runs
short of lubricants under boundary lubricated condition. We conclude that the nanostructure of interface between DLC and lubricants are very inﬂuential to the lubricated friction property.

Fig. 1. Coefﬁcients of friction under lubricated condition

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 909- 65 -

JAEA-Review 2013-039

1-1-42High Temperature Neutron Diﬀraction Study of (La0.6Sr0.4)(Co0.8Fe0.2)O3-d
Perovskite
K. Nomura (A), K. Kakinuma (B), T. Kojima (A), N. Takeichi (A), H. Kageyama (A),T.
Maekawa (C), C. Minagoshi (C), H. Miyazaki (C), and Y. Kawabata (C)(A) National Institute of Advanced Industrial Science and Technology (AIST), (B) University of
Yamanashi, (C) New Cosmos Electric Co., Ltd.
Recently, (La,Sr)(Co,Fe)O3-d perovskites
have been investigated as the cathodematerials of solid oxide fuel cells, becauseof the high electronic and high oxide-ion
conductivity [1]. However, the detailed
crystal structures under cell operation
conditions, i.e., at elevated temperatures
under oxygen partial pressures, P(O2)<= 0.21atm, have not been reported yet.
In this study, we have measured hightemperature neutron diffraction data of 40
mol% Sr- and 20 mol% Fe-doped LaCoO3,(La0.6Sr0.4)(Co0.8Fe0.2)O3-d (LSCF), atelevated temperatures, 299<=T<=1273K,
under 0.002<=P(O2)<=0.21atm, to investigate the detailed crystal structures and theoxide-ion conduction path.
Neutron diffraction measurements were
performed with a 150-detector system,HERMES [2], installed at the JRR-3M reactor in JAEA (Tokai). The neutron wave
length was 1.8204(5)A and the diffraction
data were collected in the 2 θ range from
20 to 153 deg. in step interval of 0.1 deg.
A furnace with Pt-Rh heaters installed in a
vacuum chamber was placed on the sample stage, and used for neutron-diffraction
measurements at high temperatures. The
diffraction data obtained were analyzed using the Rietveld program RIETAN-2000 [3].
The diffraction data of LSCF could beindexed assuming a trigonal symmetry(R-3c, No.167) at 299, 475, and 671K in
P(O2) = 0.21atm, or a cubic one (Pm-3m,
No.221) between 873 and 1273K under
0.002<=P(O2) <=0.21atm. The Rietveld reﬁnement result of LSFC measured at 1273K
in P(O2) = 0.002atm was as follows: Z = 1, a
= 3.9333(2)A, α = 90 deg., V = 60.854(6)Aˆ3.
The reliability factors were as follows: Rwp= 6.48%, Re = 3.43%, S = Rwp/Re = 1.89.

Figure 1 shows the reﬁned crystal structure of LSFC at 1273K in P(O2) = 0.002atm.
Oxide ions showed larger atomic displacement parameters than those of La, Sr, Co,
and Fe ions. Oxide ions also indicatedlarger thermal motion perpendicular to(Co, Fe)-O bonds. These results suggest theoxide-ion conduction in LSCF with an arc
shape path [4].
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).
[4] M. Yashima and T. Kamioka, Solid State
Ionics, 178, 1939 (2008).

Fig. 1.
Reﬁned crystal structure of(La0.6Sr0.4)(Co0.8Fe0.2)O3-d at 1273K underP(O2) = 0.002 atm. The dotted curve with arrows
denotes possible conduction path of oxide ions.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-1-43

Phonons in FCC-Fe precipitates in Cu
Kohtaro Horiguchi and Yorihiko Tsunoda
School of Science and Engineering, Waseda University, 3-4-1 Ohkubo, Shinjuku-ku, Tokyo
169-8555
An fcc-Fe is stable only at temperature
between 1185K and 1667K. However, Fe
precipitates which are grown in supersaturated Cu-Fe solid solution retain fcc structure even at room temperature. The lattices
of Fe precipitates are coherent with Cu matrix. At low temperature (T<70 K), Fe precipitates undergo a structural phase transition. The lattice structure in the low temperature phase is described by the shear
wave propagating along the [110] direction and the [1-10] polarization vector. In
related to the structural phase transition,
drastic softening of the elastic moduli C
and C11 is observed below 150 K.
The purpose of the present experiments
is two points. There are no experimental
data of phonon dispersion relation of fcc
Fe at the room temperature because of nobulk specimen. Thus, the ﬁrst purpose isto observe the phonon peaks and to determine the dispersion relations of fcc Fe atroom temperature using the coherent precipitates. If observation of phonons is possible, the second purpose is to observe thephonon softening towards the structuralphase transition.
A super-saturated Cu97Fe3 single crystal was grown by Bridgmann method. The
sample was quenched into water from 1000
C, then precipitation anneal was performed
at 600 C for 53.5 hours. Averaged precipitation particle size is estimated to be 50 nm.
Phonon measurements were performed at
the T1-1 triple axis spectrometer.
For small q regions, it was impossible
to separate the phonons of Cu matrix and
Fe precipitates. At high q regions, phonon
intensity is too weak to observe becauseof small effective volume of fcc-Fe precipitates. However, we succeeded to observe
phonon peaks of the [1 1 0] T1-branch atroom temperature. Since the elastic modu-

lus C shows softening towards the structural phase transition, to study the phonon
dispersion relation of the [1 1 0] T1 branchwould be interesting. Temperature variation of phonon peaks for fcc-Fe precipitates studied at q=0.3 is given in Fig. 1.
At low temperature, phonon peak intensity
is too weak and it is hard to discuss thephonon softening. However, phonon peakshift with temperature decreasing (hardening) between RT and 150 K is very large.
The reason is considered to be increasingof mis-ﬁtting parameter of the lattices between Cu and Fe precipitates. We would
like to discuss this point thoroughly.

Fig. 1. Fig.1 temperature variation of phonon peaksof fcc Fe precipitates studied at q=0.3.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 933- 67 -

JAEA-Review 2013-039

1-1-44

Crystal Structure Analysis of a Supramolecular Ferroelectric 55DMBP-H2ia at
Low-temperature Phase
Reiji Kumai1, Daisuke Okuyama2,3, Sachio Horiuchi1, Takahisa Arima3, Ryoji
Kiyanagi3, Yukio Noda3, and Yoshinori Tokura1,2,4
1National Institute of Advanced Industrial Science and Technology (AIST), 2Cross-CorrelatedMaterials Research Group (CMRG), ASI, RIKEN, 3Institute of Multidisciplinary Research for
Advanced Materials, Tohoku University, 4Department of Applied Physics, The University ofTokyo
Ferroelectrics have been motivated not
only by basic science but also by application because of those various utilizations
for electronics. Recently Horiuchi et al.
have reported a new ferroelectric realized
by proton dynamics in a hydrogen-bonded
chain with supramolecular structure, thecocrystal of 5,5 -dimethyl-2,2 -bipyridine(55DMBP, C12H12N2) and iodanilic acid(H2ia, C6H2O4I2) [1], in which the corrective proton motion should be playing
an important role for the development of
the ferroelectricity. Here, we report crystal structure of 55DMBP-H2ia in a lowtemperature phase obtained by the neutron
diffraction in order to make clear the more
precise hydrogen atom position.
Large single crystals of 55DMBP-H2ia (3x 1 x 10 mm3) were prepared by slow
evaporation from methanol solution. The
neutron diffraction experiments were performed at the T2-2 guide-hall of JRR-3M in
JAEA, utilizing a four-circle diffractometer
FONDER with 1.23960 neutron beam
monochromized by a Ge(311) monochromater. We used the program SHELX-97 forthe least-square ﬁtting in order to reﬁne theparameters. [2]The crystal of 55DMBP-H2ia consists of
one-dimensional chain made from O…H…
N type hydrogen bond between acid andbase molecules. Figure 1a shows the hydrogen bonded chain structure of ferroelectric phase of 55DMBP-H2ia (T = 50 K) obtained by a neutron crystal structure analysis. Lattice parameters, space group (P1),
and atomic coordinates except for hydrogen atoms, consist with those obtained by
the X-ray diffraction experiments. It can beclearly observed that there are two typesof hydrogen bonded site, a neutral O-H…
N site and a ionic O-…H-N+ site, in the
chain. From a comparison between ferroelectric structure and paralectric structure(Fig. 1b), which was determined by the previous neutron diffraction study, one canﬁnd the corrective proton motion along the
one-dimensional hydrogen bonded chain.
The alternating O-H…N and O-…H-N+
constitute a polar chain and a polar threedimensional structure. That is to say, theproton migration can be an origin of the polarization in this system.
References and notes[1] S. Horiuchi, R. Kumai, Y. Tokura,Angew. Chem. Int. Ed., 46, 3497 (2007).
[2] 55DMBP-H2ia 300K: C18H14N2O4I2, Z= 2, Triclinic P1, a = 9.996(5) , b = 8.729(2), c = 12.650(3) , alpha= 66.54(2), beta=
67.57(2),gamma= 66.45(2), V = 895.1(5) 3,
R = 0.0433 for 3115 independent reﬂections(|Fo| > 4sigma(|Fo|)).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 937- 68 -

JAEA-Review 2013-039

1-1-45

Crystal Structure of Lithium Battery Electrode Materials with Tunnel Structure
N. Kijima(A), J. Akimoto(A), K. Kataoka(A,B)(A) National Institute of Advanced Industrial Science and Technology (AIST), (B) University ofTsukuba
A great deal of research into the application of a-MnO2 as an electrode material for lithium-ion batteries has been conducted because a-MnO2 has large (2 × 2)
tunnels presenting a privileged pathway
for Li ion diffusion [1-3]. The a-MnO2 electrode can be intercalated in lithium cells
at about 3 V, and the initial discharge capacity exceeds 200 mAh/g. To clarify the
structural properties of a Li inserted aMnO2 specimen, neutron diffraction investigations have been made in this work.
A well-crystallized a-MnO2 specimen
was prepared by oxidation of MnSO4 withozone gas in H2SO4 solution at 353 K. A
Li inserted a-MnO2 specimen was obtainedby soaking the parent a-MnO2 powder in amixed solution of 0.1 mol/dm3 LiOH and
0.1 mol/dm3 LiNO3.
Neutron powder diffraction data weretaken at room temperature on the HERMES
powder diffractometer installed at the JRR3M research reactor of the Japan Atomic
Energy Agency. Incident neutrons with aﬁxed wavelength of 1.8204(5) angstroms
were obtained by a vertically focusing (331)
Ge monochromator. The powder diffraction data were measured over a 2 theta
range of 7-157 degrees with a step intervalof 0.1.
The diffraction data were analyzed by
the Rietveld method with RIETAN-2000,
and the nuclear scattering density distribution of specimens were visualized by the
maximum-entropy-method based pattern
ﬁtting.
Figure 1 depicts the preliminary result of
the nuclear scattering density distributionof Li inserted a-MnO2 specimen. This image clearly shows the Li and O atoms in thetunnel space.
The parent a-MnO2 specimen showeda poor discharge property although

no cationic residues or residual H2O
molecules remained in the tunnel space. In
contrast, the Li inserted a-MnO2 specimen
showed a good charge-discharge property
as the cathode. These facts suggest that thepresence of stabilizing O atoms within the(2 × 2) tunnel is necessary to facilitate thediffusion of Li ions during cycling.
References[1] N. Kijima, T. Ikeda, K. Oikawa, F. Izumi,
Y. Yoshimura, J. Solid State Chem. 177(2004) 1258.
[2] N. Kijima, Y. Takahashi, J. Akimoto,J. Awaka, J. Solid State Chem. 178 (2005)
2741.
[3] N. Kijima, Y. Sakata, Y. Takahashi, J. Akimoto, T. Kumagai, K. Igarashi, T. Shimizu,
Solid State Ionics 180 (2009) 616.

Fig. 1. Nuclear scattering density distribution imageof the Li inserted a-MnO2 specimen.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 957- 69 -

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JAEA-Review 2013-039

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1. Neutron Scattering- 71 -

2 Magnetism

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JAEA-Review 2013-039

1-2-1
Magnetic Bragg Peaks of Quasi-One-Dimensional Antiferromagnets
Cu6 Ge6 O18 -xD2 O (x = 0, 6)
M. Hase, N. Terada, H. S. Suzuki, H. Kitazawa, K. Ozawa, K. Kaneko1 , N. Metoki1 ,M. Matsuda1 and K. Kakurai1
1

National Institute for Materials Science (NIMS), 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan
Japan Atomic Energy Agency (JAEA), 2-4 Shirakata Shirane, Tokai, Naka, Ibaraki 319-1195, JapanThe spin systems of insulating cuprates
Cu6 Ge6 O18 -xD2 O (x = 0 − 6) are spin1/2 Heisenberg chains with ﬁrst- and secondnearest-neighbor antiferromagnetic (AF) exchange interactions.1) The space group is R3̄
(No. 148).2) Helical spin-1/2 chains of Cu
are formed parallel to the c axis. Each chain
has three Cu ions in the unit cell. Magnetic long-range order appears below TN . The
value of TN /Tmax decreases with decrease inx from x = 6, while it is nearly constant
below x = 1.54. Here, Tmax is temperature where the magnetic susceptibility has
a broad maximum. At x = 1.54, TN /Tmax
jumps abruptly from 0.23 to 0.39, and twomagnetic transitions are seen. The jump indicates that magnetic long-range orders at
x < 1.54 and x > 1.54 belong to essentially diﬀerent phases. The diﬀerence, however, has not been unveiled. Accordingly, we
performed neutron-diﬀraction measurementsof powders with x = 0 or 6 using the TAS-2(the wave length λ = 2.444 Å) and MUSASI(λ = 2.474 Å) spectrometers to investigate
magnetic structures.
Figure 1 shows diﬀraction patterns of
Cu6 Ge6 O18 -6D2 O.3) As indicated by arrows,
we can see a resolution-limited magnetic
Bragg peak in each ﬁgure below TN . We
could ﬁnd two magnetic Bragg peaks in eachsample. The index (h, k, l) of the scatteringvector Q is (2, 1, −0.5)hex and (1, 2, 0.5)hex
for the low-angle peak and (3, 1, 0.5)hex and(1, 3, −0.5)hex for the high-angle one. We
adopt the hexagonal unit cell. The l value ishalf integer. Therefore, the spin arrangement
is collinear AF in each chain.

AF or ferromagnetic. Here, we assume thatthe ordered spins are parallel to the c axis, because the spin is almost parallel to the c axis
in the AF long-range order in isostructuralCu6 Si6 O18 -xH2 O (x = 0, 6).4, 5) The calculated SCSs in the case that Ja is AF are consistent with the experimental results.
4

装置：TAS-2(T2-4)

8 8 933 *   

12
(*
'/0
- .    
+( ,
!:9
( '*)
&'
!"#$
5 6 7 
!%



;




4
33 *
8 8:9
1>(*'/0  8;  
-.
+( ,
!:9
( '*)
& '    
!

"



"

#

<

"
5 =7
!%Figure 1: Diﬀraction patterns of Cu6 Ge6 O18 -6D2 O.

References

We calculated scattering cross sections(SCSs) of magnetic Bragg peaks when thenearest-neighbor interchain interaction (Ja ) is
原子炉：JRR-3

 

1) M. Hase, K. Ozawa and N. Shinya : ”Phys. Rev.
B”, 68, pp. 214421 (2003).
2) H.-J. Brandt and H. H. Otto : ”Z. Kristallogr.”,
212, pp. 34 (1997).
3) M. Hase, N. Terada, H. S. Suzuki, H. Kitazawa,K. Ozawa, K. Kaneko, N. Metoki, M. Matsuda
and K. Kakurai : ”J. Phys.: Conference Series”,
150, pp. 042051 (2009).
4) M. Wintenberger, G. André and M. F. Gardette: ”Solid State Commun.”, 87, pp. 309 (1993).
5) E. L. Belokoneva, Y. K. Gubina, J. B. Forsythand P. J. Brown : ”Phys. Chem. Minerals”, 29,
pp. 430 (2002).

分野：中性子散乱（磁性）- 73 -

JAEA-Review 2013-039

1-2-2
Spherical Neutron Polarimetry Analysis in the Ferroelectric Phase of theMagnetoelectric Multiferroic CuFe1−y Gay O2
N. Terada1,3 , T. Nakajima2 , S. Mitsuda2 , M. Matsuda3 , K. Kakurai3 and H. Kitazawa1
1

National Institute for Materials Science, Tsukuba, Ibaraki 305-0047
Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601
3
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Recently, as one of magnetoelectric multiferroics, CuFeO2 has been intensively studied
for understanding the microscopic mechanism
regarding the magneto-ferroelecticity.1, 2)
There has been several theories to explain
ferroelectricity in multiferroics. One of themechanisms was proposed for explaining theferrelectricity in CuFeO2 , which originatesfrom Fe 3d-O 2q hybridization with thespin-orbit coupling.3) For the veriﬁcation of
the mechanism, the detail magnetic structural determination was strongly required.
Although the previous unpolarized neutron
diﬀraction experiments have determined themagnetic structure to be proper helical one,4)
its ellipticity has not been clariﬁed. Our
recent study demonstrated that nonmagnetic
Ga doping leads to the ferroelectric phasewith the single magnetic modulation wave
number.5)
This time, we have performed the sphericalneutron polarimetry analysis on the ferroelectric phase of CuFe0.963 Ga0.037 O2 at the tripleaxis spectrometer TAS-1 with the CRYOPAD
option installed at JRR-3 in JAEA. In thisexperiment, we can measure the neutron polarization matrix with three dimensional components for incident and scattered neutrons.
Figure 1 shows scattering vector (of themagnetic reﬂection) dependence of the neutron polarization matrix term Pyy (= −Pzz ).
The experimental data was reﬁned by leastsquare analysis, where the reﬁned parameteris the ellipticity (μ11̄0 /μc ). μc and μ11̄0 mean
the momentum amplitude in the c and 11̄0
spin components, respectively. As clearly seenin this ﬁgure, the reﬁned ellipticity is not 1.0
but about 0.9.
For the veriﬁcation of the theory above
mentioned,3) the understanding of the spa原子炉：JRR-3

装置：TAS-1(2G)

0.4

[001]

(a)

μa/μc=0.895
T=1.4 K

0.2
[1-10]

0.0

Pyy, -Pzz

2

-0.2
-0.4
-0.6
μ μ
μ μ

-0.8
-1.0

0

20

40

60

80

ω [deg]Figure 1: Comparison of the calculated curves andexperimental data for the neutron polarization matrix
terms, Py,y and −Pzz . ω is the relative angle between
the hexagonal [110] axis and the scattering vector ofeach magnetic reﬂection. The dashed and solid lines
denote the calculated curves for the ellipticity of 1.0
and 0.895, respectively.

cial modulation of the electric dipole moments
coupled with magnetic moments, which waspredicted to be with two times larger wave
number than the magnetic one, is strongly desired. The presently determined elliptic magnetic structure will help understanding the
microscopic coupling between spin and electric dipole moment.
References
1) T. Nakajima et al. :“Phys. Rev. B”, 78, pp. 024106(2008).
2) T. Nakajima et al. :“Phys. Rev. B”, 78, pp. 214423(2009).
3) T. Arima et al. :“J. Phys. Soc. Jpn.” 76, pp.
073702 (2007)
4) T. Nakajima et al. :“J. Phys. Soc. Jpn.”, 76, pp.
043709 (2007).
5) N. Terada et al. :“Phys. Rev. B”, 78, pp. 014101(2008).

分野：中性子散乱（磁性）- 74 -

JAEA-Review 2013-039

1-2-3
Magnetic and Structural Phase Transitions of RbFeBr3
Y. Nishiwaki, K. Kakurai1 and T. Kato2
Department of Physics, Tokyo Women’s Medical University, Shinjuku-ku, Tokyo 162-8666
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
2Faculty of Education, Chiba University, Inage-ku, Chiba 273-8522

ature dependence of this peak height showsan anomaly at TC . The antiferromagnetic
phase transitions occur at TN1 = 5.5 K andTN2 = 2.0 K.4) Therefore, ferroelectricity andspin order are coexisted below TN1 . The temperature dependence of the ( 13 13 1) and (1 1 1)
magnetic peak heights are shown in Fig. 1.
The ( 13 31 1) peak is observed below TN1 but
the (1 1 1) peak is observed only below TN2 .
The spin structures at TN2 < T < TN1 andT < TN2 are determined as the partial disordered and the triangular ones, respectively.
We observed the small spontaneous magnetization perpendicular to the c-axis below TN1 .
3

12x10

10
1500

装置：TAS-2(T2-4)

TN1

8 (1/3 1/3 1)
6

1000

4

(1 1 1)

500

2

TN2

0
0

2

0
4

6

8

Temperature [K]Figure 1: Temperature dependence of ( 13 31 1) (leftaxis) and (1 1 1) (right axis) neutron diﬀraction peakheights of RbFeBr3 .

References

RbFeBr3 undergoes successive structuralphase transitions at Tst1 = 109 K and Tst2 =TC = 39.5 K. Below TC , ferroelectricity exhibits. In the present measurements, ( 13 31 2)
peak was observed below Tst1 . The temper原子炉：JRR-3

2000

RbFeBr3

Counts [/20s]

Among magnetic compounds with the
ABX3 chemical formula, the CsNiCl3 -type
antiferromagnets take the perovskite-likestructure with hexagonal close packed AX3
layers, in which face-sharing BX6 octahedra
run as forming a -BX3 - chain along the c-axis.
Their nearest-neighbor magnetic B 2+ ionson the c-plane form a triangular lattice andgive rise to spin frustration. There are several compounds, such as KNiCl3 , RbMnBr3 ,TlCoCl3 and RbCoBr3 , crystal structuresof which are distorted from the prototype
CsNiCl3 -structure through structural phasetransitions. The lattice distortions are characterized by the shifts of the chains either upwards or downwards along the c-axis. The
spin frustration is released by the distortion.
In a certain case, breaking of inversion symmetry by the lattice distortion is accompaniedwith and the crystal structure is polar. We
call these crystals members of the KNiCl3 family. Most KNiCl3 -family compounds exhibit ferroelectricity at certain phases. We
have been interested in how these lattice distortions and electric polarization aﬀect themagnetism of those crystals and vice versa.
In past, we determined the magnetic and crystal structures of RbMnBr3 1) (Heisenberg spinwith easy plane anisotropy), TlCoCl3 2) (Isingspin), and RbCoBr3 3) (Ising spin) throughthe neutron diﬀraction measurements. In thepresent study, we performed the single-crystal
neutron diﬀraction measurements in RbFeBr3
which is one of the KNiCl3 compounds. The
magnetic phase transitions of RbFeBr3 are described as the XY spin systems.

Counts [/5s]11) T. Kato: J. Phys. Soc. Jpn. 71 (2002) 300.
2) Y. Nishiwaki, T. Kato, Y. Oohara, A. Oosawa, N.
Todoroki, N. Igawa, Y. Ishii, and K. Iio: J. Phys.
Soc. Jpn. 75 (2006) 034707.
3) Y. Nishiwaki, T. Nakamura, A. Oosawa, K. Kakurai, N. Todoroki, N. Igawa, Y. Ishii, and T. Kato:
J. Phys. Soc. Jpn. 77 (2008) 104703.
4) K. Adachi, K. Takeda, F. Matsubara, M. Mekata
and T. Haseda: J. Phys. Soc. Jpn. 52 (1983) 2202.

分野：中性子散乱（磁性）- 75 -

JAEA-Review 2013-039

1-2-4
Crystal Structure Analysis and Magnetic Properties of Multiferroic System
Ni3(1−x) Cu3x V2 O8
T. Kai, Y. Yasui, M. Sato, H. Fukazawa1 , N. Igawa1 , and K. Kakurai1
Department of Physics, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8602
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Ni3 V2 O8 is an insulating system with Ni2+
spins (spin S=1) arranged in a kagomé staircase or in a buckled kagomé plane. The
system exhibits three magnetic transitionsat temperatures Tc1 =9.1 K, Tc2 =6.3 K and
Tc3 =3.9 K. In the region Tc2 < T < Tc1 ,the spins have a sinusoidally modulated incommensurate structure with the spin direction along a and the modulation vector alonga (HTI phase). In the region Tc3 < T <Tc2 , they have a helically modulated structure within the ab-plane with the modulation vector along a (LTI phase). Below Tc3 ,the weak spin canted ferromagnetic structure
is realized with a commensurate modulation
vector along a (C phase). The multiferroic
behavior or the coexistence of magnetic andferroelectric orders can be found in the region
Tc3 < T < Tc2 .1) The helical magnetic structure originates from the competing nearest
neighbor(J1 ) and next nearest neighbor(J2 )interactions. For this system, impurity doping eﬀects has been studied, because the Zn,
Co, Mn and Cu substitution for Ni may
change the magnetic and dielectric behaviors,and present information on the mechanismof the multiferroic phenomenon. Anotherinteresting view point of the system is theexistence of the successive magnetic transitions, because the system has the geometricalfrustration inherent in the crystal structure.
First, we have carried out measurements ofthe magnetization, speciﬁc-heat and dielectric
properties of Ni3(1−x) M3x V2 O8 (M=Zn, Co,
Mn and Cu). For Ni3(1−x) M3x V2 O8 (M=Zn,
Co and Mn), all the three transition temperatures (Tc1 , Tc2 and Tc3 ) are found to monotonically decrease with increasing x. In contrast, for Ni3(1−x) Cu3x V2 O8 , Tc3 was foundto increase and Tc1 and Tc2 were found to
decrease (The C phase is stabilized). In thesamples with x > 0.1, the LTI phase is notfound and the ferroelectricity does not exist.
The crystal system changes from orthorhombic to monoclinic ones at around x=0.25 withincreasing x. Next, to obtain detailed infor原子炉：JRR-3

装置：HRPD(1G)

mation on the crystal and magnetic structures of Ni1.5 Cu1.5 V2 O8 , the powder neutron
diﬀraction measurements have been carriedout at 50K and 3K by using the high resolution powder diﬀractometer (HRPD) installedat JRR-3 of JAEA in Tokai. The horizontal collimations were 12’-40’-6’ and the neutron wavelength was 1.8231 Å. We have carried out the Rietveld analysis on the data
at 50 K (paramagnetic phase), and the data
can be almost explained by using the spacegroup P 21 /c, where a=11.4369 Å, b=8.1350
Å, c=6.0880 Åand β = 89.01◦ . A schematic ofthe (Ni,Cu)O6 octahedron is shown in the upper part of the ﬁgure. The z’ axis of the local
coordinates expands by the Cu-doping, whichis considered to be due to the Jahn-Teller effect of the Cu2+ ions. The lower part of theﬁgure shows the view of the cut plane parallelto the ab-plane of the one-dimensional chainsof edge-sharing (Ni,Cu)O6 octahedra. It indicates that the doped Cu2+ ions disconnect thesome exchange interactions J1 and J2 . The
results seem to be related to the stability of
the C phase at low temperature. We have determined the magnetic structure at T =3 K of
Ni1.5 Cu1.5 V2 O8 ; The characteristics of the ordering pattern are similar to those of C phaseof Ni3 V2 O8 except for the easy axis directionof spins.

References
1) G. Lawes et al.; Phys. Rev. Lett. 95 (2005) 087205.

分野：中性子散乱（磁性）- 76 -

JAEA-Review 2013-039

1-2-5
Studies of Multiferroic System of LiCu2 O2 -Magnetic Structures of Two Ordered
Phases with Incommensurate ModulationsK. Sato, Y. Yasui, T. Moyoshi,Y. Kobayashi, M. Sato, and K. Kakurai1
Department of Physics, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8602
1
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

By the combined work of neutron diﬀraction and 7 Li-NMR, the three dimensional
magnetic structures of the multiferroic system LiCu2 O2 , which has four chains (ribbon
chains) of edge-sharing CuO4 square planes
in a unit cell have been determined.1,2) In
the course of the studies, we have ﬁrst realized that for the complete determination ofits magnetic structures, it is insuﬃcient toreproduce, by choosing a set of parameters,
only one kind of experimental data, because
we have to use a number of parameters to
describe the modulated magnetic structuresof the four ribbon chains. We have therefore
applied experimental means of 7 Li-NMR andneutron magnetic scattering on single crystal samples, trying to consistently explain thedata of these methods. The neutron experiments have been carried out on a single crystal of 7 LiCu2 O2 by using the triple axis spectrometer TAS-1 installed at JRR-3 of JAEA
in Tokai. To avoid the large neutron absorption of Li nuclei, we used the 7 Li isotope inthe measurements. The horizontal collimations were 40’-40’-80’-open, and the neutron
wave length was 2.359 Å. The 002 reﬂectionof Pyrolytic graphite (PG) was used as the
monochromator. A PG ﬁlter was placed after
the second collimator to suppress the higherorder contamination. The crystal was oriented with the [100] and [010] axes, in one
case, and the [102] and [010] ones, in anothercase, in the scattering plane. The size of thecrystals was ∼ 18 × 16 × 1 mm3 , and the integrated intensities of 20 nonequivalent magnetic Bragg reﬂections were measured. In theanalyses of the data, the anisotropic magnetic
form factor for Cu2+ ions deduced from thex2 − y 2 orbit was used, and the absorption
corrections considering the shape of the single
crystal were made. First, we have conﬁrmedthat the system has two successive magnetictransitions at TN1 ∼ 24.5 K and TN2 ∼ 22.8 K.
In the temperature region between TN1 andTN2 , the magnetic structure has been foundto be a sinusoidally modulated incommensu原子炉：JRR-3

装置：TAS-1(2G)rate one. At T < TN2 , an ellipsoidal helicalspin structure with the incommensurate modulation has been found (Fig. 1). As statedabove, by combining the NMR and neutrondata, we have succeeded in the determinationof detailed parameters related to the modulation amplitudes, helical axis vectors and relative phases of the modulations of four ribbon
chains, which can reproduce both the NMR
and neutron results, in the two magneticallyordered phases. This ﬁnding of the rather precise magnetic structures enables us to discuss
the relationship between the magnetic structure and the multiferroic nature of the present
system in zero magnetic ﬁeld, and open a way
how to understand the reported electric polarization under the ﬁnite magnetic ﬁeld.

ºFigure 1: Magnetic structure of a CuO2 ribbon chain
in LiCu2 O2 below TN2 is shown schematically. There
are four chains in a unit cell and the relative phasesof their modulations have also determined.

References
1) Y. Kobayashi, K. Sato, Y. Yasui, T. Moyoshi,
M. Sato, and K. Kakurai: J. Phys. Soc. Jpn. 78(2009) No. 8.
2) Y. Yasui, K. Sato, Y. Kobayashi, and M. Sato: J.
Phys. Soc. Jpn. 78 (2009) No. 8.

分野：中性子散乱（磁性）- 77 -

JAEA-Review 2013-039

1-2-6
Crystal-Field Study of Clathrate Rare-Earth Compounds Ce3 Pd20 (Si1−x Gex )6
with Multi-Polar Ordering
H. Kitazawa, N. Terada, Y. Tsuchiya, Y. Kawamura, A. Kikkawa, A. Dönni, O. Sakai, M.
Matsuda1 , K. Kakurai1 , Y. Nemoto2 and T. Goto2
National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047
Japan Atomic Energy Agency (JAEA), 2-4 Shirakata Shirane, Tokai, Naka, Ibaraki 319-1195
2
Graduate School of Science and Technology, Niigata University, Niigata 950-2181

The rare-earth clathrate compounds
Ce3 Pd20 X6 (X = Si, Ge) crystallize in the
C6 Cr23 - type structure belonging to the spacegroup symmetry Fm3̄m. In this structure, Ce
atoms occupy two diﬀerent crystallographic
sites, 4a and 8c, both with a cubic point
symmetry Oh and Td , respectively. The
heavy fermion compounds Ce3 Pd20 Si6 1)
and Ce3 Pd20 Ge6 2) undergo successive
quadrupole ordering (below TQ = 0.5 K and
1.2 K, respectively) and antiferromagnetic
ordering (below TN = 0.31 K and 0.7 K,
respectively). The inelastic neutron scattering (INS) experiment 3) revealed that the
crystalline ﬁeld (CEF) scheme of Ce ions forboth sites in Ce3 Pd20 Ge6 consists of a Γ8
quartet ground state and a excited Γ7 doublet
state, with a splitting energy of 4.0 meVat the 8c-site and 5.2 meV at the 4a-site.
Very recently, however, we observed only one
well-deﬁned excitation of 3.7 meV at 5 K in
Ce3 Pd20 Si6 , In order to investigate the originof the single CEF excitation in Ce3 Pd20 Si6 ,we have performed INS experiments in thepseudo-ternary systems Ce3 Pd20 (Si1−x Gex )6
using TAS2 spectrometer of JRR-3 in Tokai.
The INS spectrum of polycrystalline samples Ce3 Pd20 (Si1−x Gex )6 (x = 0, 0.1 0.3, 0.5
1) are shown in Fig. 1. Our data for x= 1 demonstrates a main peak at 4.0 meV(peak A) and a shoulder peak at 5.3 meV(peak B) which is consistent with the previous
data 3) . With decreasing x value, the peak B
becomes unclear and the shape of the combined peak (A and B) remains asymmetric.
In order to decompose the overlapping peaks
into two Gaussian peaks, we assumed that thebackground forms a linear function and theratio of their integrated intensity is equal to
原子炉：JRR-3

装置：TAS-2(T2-4)

2 : 1, which corresponds to the ratio of thenumber of Ce ions on the 8c- and 4a-site, respectively. We could ﬁt all the experimental
data by this simple model as shown by brokenlines in Fig. 1. The x dependence of peak A
is very weak. In contrast, with decreasing x
value, the amplitude of peak B strongly decreases and the peak width increases. The
CEF splitting at the 4a-site is aﬀected by replacement of Si atoms for Ge atoms. It suggests that the characteristic of 4f electrons at
4a-site changes from localized state to itinerant or well-hybridized state.
Ce3Pd20(Si1-xGex)6 , 5K, EA = 13.7 meV
A

200

B

100
Neutron Intensity ( counts/1,200,000Mon )

1

0
200

x=1

x = 0.51000200

x = 0.31000200
x = 0.1

100
0
200

x=0
100
0
-2

0

2
4
6
8
Energy transfer ( meV )10

12

Figure 1: INS spectrum of Ce3 Pd20 (Si1−x Gex )6 (x =0, 0.1 0.3, 0.5 1) at 5 K.

References
1) A. M. Strydom, et al. :“J. Phys. Conf. Ser.”, 51,
pp. 239-242 (2006).
2) J. Kitagawa, et al. :“Phys. Rev. B”, 53, pp. 51015103 (1996).
3) L. Keller, et al. :“Physica B”, 259-261, pp. 336337 (1999).

分野：中性子散乱（磁性）- 78 -

JAEA-Review 2013-039

1-2-7
Enhancement of the Two-Dimensional Spin Correlations in Ag doped CuCrO2
R. Kajimoto, M. Matsuda1 , T. Kishimoto2 , K. Uto2 , T. Hokazono2 and T. Okuda2
J-PARC Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
2
Department of Nano-structures and Advanced Materials, Kagoshima University, Kagoshima 890-0065
1

Figure 1(a) shows powder diﬀraction patterns of Cu0.85 Ag0.15 CrO2 at 6, 15, and 100 K.
At 6 K, 3D magnetic Bragg peaks are observed at (q, q, 0), (q, q − 1, 0), (q − 1, q, 2),(q, q, 3), etc. with q ∼ 1/3. By investigating
the peak positions in detail, we found that q
is slightly diﬀerent form 1/3 and it was 0.328.
Interestingly, this incommensurability is almost same as that reported in the end compound, AgCrO2 (0.327).3) At a temperature
just above TN (15 K), the Bragg peaks disappear, but intense broad scattering remains
around (q, q, 0). The proﬁle of this broad scattering has a skewed structure, which is a typical proﬁle of a 2D system. The 2D correlations were also evidenced by the fact that
原子炉：JRR-3

装置：TAS-2(T2-4)

this scattering proﬁle can be well ﬁtted to
the Warren function4) , as shown by a broad
solid line in Fig. 1(a). As a comparison, we
also performed similar measurements on the
non-doped (x = 0) sample [Fig. 1(b)]. The
non-doped sample also shows the 2D scattering just above TN , but the ratio of the 2D
scattering intensity to the 3D Bragg peaks ismuch reduced compared with x = 0.15. These
results clearly indicate that 2D character inthe magnetic correlations is much enhancedby the Ag doping.
Cu1-xAgxCrO2Intensity (counts/30sec)

600

Intensity (counts/30sec)

CuCrO2 has a delafossite structure, whereedge-shared CrO6 octahedral layers and Cu
layers stack alternatively. Since Cr3+ ionshave S = 3/2 spins and they form a twodimensional (2D) triangular lattice, CuCrO2
attracted attention as one of the 2D antiferromagnet. In spite of the layered crystal structure, the spins of Cr ions have ﬁnite interplanar coupling, which yields three-dimensional(3D) magnetic ordering below TN = 26 K.
The magnetic structure is a 120◦ structurewith the spins lying on the ac plane.1) Recently, however, it was revealed by a speciﬁc heat study that substitution of Cu+ ion(3d10 ) with Ag+ ion (4d10 ) induces crossoverfrom 3D to 2D low-energy magnetic excitations in addition to the decrease of TN .2) In
the present study, we studied Cu1−x Agx CrO2
by neutron diﬀraction to conﬁrm the dimensional crossover of magnetic correlations by
Ag doping. The sample was powders of x = 0
and 0.15 (TN = 14 K). The neutron diﬀraction measurements were performed using thetriple-axis spectrometer TAS-2 with an incident energy Ei = 14.7 meV.

(a) x=0.15
500
400

6K
15K
100K
Warren func.

300
200
Al

100
1200
1000

(b) x=0

5K
30K
100K

800
600
400
200
20

Al

30

40

50

60

70

Scattering Angle (deg)Figure 1: Powder neutron diﬀraction patterns of (a)Cu0.85 Ag0.15 CrO2 and (b) CuCrO2 .

References
1) H. Kadowaki et al., J. Phys.: Condens. Matter 2,4485 (1990).
2) T. Okuda et al., J. Phys. Soc. Jpn. 78, 013604(2009).
3) Y. Oohara et al., J. Phys. Soc. Jpn. 63, 847 (1994).
4) B. E. Warren, Phys. Rev. 59, 693 (1941).

分野：中性子散乱（磁性）- 79 -

JAEA-Review 2013-039

1-2-8
Dynamical Character of the Two-Dimensional Spin Correlationsin Ag doped CuCrO2
R. Kajimoto, M. Matsuda1 , T. Kishimoto2 , K. Uto2 , T. Hokazono2 and T. Okuda2
J-PARC Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
2
Department of Nano-structures and Advanced Materials, Kagoshima University, Kagoshima 890-0065
1

Figure 1 (a) shows temperature dependenceof elastic scattering proﬁles of the magnetic
scatterings. In contrast to the result at TAS2,3) the 2D scattering at 15 K is much reduced. The diﬀerence in the 2D scattering intensity can be attributed to the diﬀerence inthe energy resolution (ΔE = 1.2 meV at TAS2 and 0.2 meV at LTAS). If the 2D scattering
is dominated by an inelastic component, theelastic scattering intensity is apparently reduced in the high-energy-resolution measurement at LTAS. The dynamical character was
more directly evidenced by an energy scan,
原子炉：JRR-3

装置：LTAS(C2-1)

Intensity (counts/5x106 monitor)

Intensity (counts/5x106 monitor)

which is shown in Fig. 1(b). We observedthat the magnetic scattering spreads to theenergy of ∼0.8 meV. From the present study,
we conﬁrmed that the 2D magnetic correlations in Cu0.85 Ag0.15 CrO2 consists mostly ofdynamical component.
Cu0.85Ag0.15CrO2

600

(a)

2.8K
15K
50K

500
400
300
200
100
1.2

1.4

1.6

Q (Å-1)1.8

2

Cu0.85Ag0.15CrO2

200

(b)

T=15K

150

Q=1.4Å-1

60

Q=1.9Å-1
100

40

50

20

0
-0.5

0

0.5

Energy (meV)

1

0
1.5

Intensity (counts/3x106 monitor)

Delafossite oxide CuCrO2 is one of thetwo-dimensional (2D) triangular antiferromagnets. In this compound, S = 3/2 spins of
Cr3+ ions form a 2D triangular lattice. The
Cr layers are separated from each other by Culayers. However, the coupling between the
Cr layers is strong enough to yield a threedimensional (3D) magnetic ordering with a120◦ structure below TN = 26 K.1) Recently,
however, it was revealed by a speciﬁc heatstudy that substitution of Cu+ ion (3d10 ) with
Ag+ ion (4d10 ) induces crossover from 3D
to 2D low-energy magnetic excitations.2) As
mentioned elsewhere, we have performed neutron diﬀraction measurements on the powder
sample of Cu0.85 Ag0.15 CrO2 using the tripleaxis spectrometer TAS-2, and conﬁrmed thatthe 2D scattering at a temperature just above
TN is much enhanced compared with thenon-doped compound.3) In the present study,
we performed high-energy-resolution neutron
scattering measurements on a powder sampleof Cu0.85 Ag0.15 CrO2 to clarify the character ofthe 2D magnetic correlations. The measurements were performed using the triple-axis
spectrometer LTAS with a scattered neutronenergy Ef being ﬁxed at 3.5 meV.

Figure 1: (a) Powder neutron diﬀraction patterns of
Cu0.85 Ag0.15 CrO2 at 2.8, 15, and 50 K. (b) Energy
scan proﬁles of Cu0.85 Ag0.15 CrO2 at 15 K measured
at Q = 1.4 Å−1 and 1.9 Å−1 . The latter proﬁle represents the energy resolution.

References
1) H. Kadowaki et al., J. Phys.: Condens. Matter 2,4485 (1990).
2) T. Okuda et al., J. Phys. Soc. Jpn. 78, 013604(2009).
3) R. Kajimoto et al., this issue.

分野：中性子散乱（磁性）- 80 -

JAEA-Review 2013-039

1-2-9
Spin Correlations in a Frustrated Spinel Antiferromagnet LiCrMnO4
M. Matsuda, Z. Honda1 , H. Aruga Katori2 , H. Takagi2 , H. Ueda3 , Y. Ueda3 , H. Mitamura3
and K. Kindo3
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
3
The Institute for Solid State Physics, The University of Tokyo, Kashiwa, Chiba 277-8581

Geometrically frustrated antiferromagnets
show interesting phenomena originating fromthe macroscopic ground state degeneracy.
The pyroclore lattice, in which corner-sharing
tetrahedra of the magnetic ions are linked
three-dimensionally, is known as highly frustrated magnetic system.
LiCrMnO4 has the spinel structure, inwhich the Cr3+ and Mn4+ moments with
S=3/2 are randomly located at the cornersof the tetrahedron in pyrochlore lattice. 1) It
shows a spin-glass behavior below Tg ∼13 K
suggested from the magnetic susceptibility experiments. In order to clarify the magnetic
properties from the microscopic point of view,
we performed neutron scattering experiments
on TAS-2. It was found that short-range
spin correlations with characteristic Q ∼0.6
and 1.6 Å−1 develop at low temperatures, as
shown in Fig.1. The spin correlation with
Q ∼1.6 Å−1 (phase I) is explained by the antiferromagnetic ﬂuctuations originating fromthe hexagonal spin clusters, which is proposed
in ZnCr2 O4 above TN . 2) Although the origin of the spin correlation with Q ∼0.6 Å−1(phase II) is still unknown, the spin correlation probably originates from a new magnetic
state in highly frustrated pyrochlore lattice.
LiCrMnO4 also shows an interesting behavior in magnetic ﬁeld. Magnetization in
LiCrMnO4 gradually increases and saturates
at ∼1/2 of the full moment (3μB ). This phenomenon is similar to the half-magnetization
plateau observed in ACr2 O4 (A: Cd and Hg),
which originates from a strong spin-latticecoupling. 3) We performed neutron scatteringexperiments in LiCrMnO4 in magnetic ﬁeld
up to 10 T to clarify the origin of the plateaulike state. It was found that the magnetic
原子炉：JRR-3

装置：TAS-2(T2-4)

peak at Q ∼0.6 Å−1 is suppressed with increasing magnetic ﬁeld although the magnetic
peak at Q ∼1.6 Å−1 is robust. This result
suggests that the saturation of the magnetization is not related with the spin-latticecoupling as in ACr2 O4 but spins in phase II
ﬁrst align ferromagnetically in low magnetic
ﬁeld. This indicates that the magnetic interactions in phase II are relatively small, suggesting that the phase II is formed by furtherneighbor interactions.

Figure 1: Neutron diﬀraction patterns at 4, 20 and 100
K in LiCrMnO4 . The background intensity measured
at 200 K is subtracted.

References
1) M. Tachibana et al.: Phys. Rev. B 66, 092406(2002).
2) S.-H. Lee et al.: Nature 418, 856 (2002).
3) H. Ueda et al.: Phys. Rev. Lett. 94: 047202 (2005);
H. Ueda et al.: Phys. Rev. B 73, 094415 (2006);
M. Matsuda et al.: Nature Phys. 3, 397 (2007).

分野：中性子散乱（磁性）- 81 -

JAEA-Review 2013-039

1-2-10Magnetic Field-Induced Transitions in the Spinel GeCo2 O4
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 shows an antiferromagnetic ordering with a characteristic wave
vector of QM =(1/2, 1/2, 1/2) below TN ∼21
K accompanied with a structural phase transition from cubic to tetragonal symmetry. Recently, magnetic properties of GeCo2 O4 in
magnetic ﬁeld were studied by magnetization measurements. 1, 2) It was reported thatmagnetization in polycrystalline GeCo2 O4 exhibits an anomaly at H=4.25 and 9.70 T,
which correspond to magnetic transitions. 1)
The magnetization measurements using single crystal also show magnetic phase transitions at H ∼4.5 and 10 T, depending on themagnetic ﬁeld directions. 2) The anomaly at
H ∼4.5 T is observed only when the ﬁeld isapplied along the (110) and (111) directions.
In order to understand the magnetic interactions in GeCo2 O4 , it is important to determine the magnetic structure in the magnetic
ﬁeld-induced phases.
In order to clarify the magnetic structure inmagnetic ﬁeld, we performed neutron diﬀraction experiments on TAS-2 using polycrystalline sample of GeCo2 O4 . We ﬁrst conﬁrmed that the magnetic structure in zeromagnetic ﬁeld is consistent with that reported
previously. 1) The magnetic structure is basically the same as that in GeNi2 O4 below TN2 ,in which the spin arrangement is ferromagnetic in the kagomé and triangular planes andantiferromagnetic between the kagomé andtriangular planes. 3) With applying magnetic
ﬁeld, the magnetic Bragg intensities change
drastically, originating from both change inmagnetic structure and orientation of magnetic domains, as shown in Fig. 1. We foundthat the eﬀect of the domain orientation is
not so distinct at higher temperatures andperformed Rietveld reﬁnement analysis. Fortunately, an overall feature of the magnetic
原子炉：JRR-3

装置：TAS-2(T2-4)

structure in magnetic ﬁeld could be determined even with powder sample. The spin arrangement between the triangular planes becomes ferromagnetic around 4 T and the spinarrangement between the kagomé planes also
becomes ferromagnetic gradually above ∼4 T.
Finally, all the spins align ferromagneticallyalong the ﬁeld direction at ∼10 T. These results suggest that the kagomé and triangular planes become more decoupled in magnetic ﬁeld, which is similar to the behaviorof GeNi2 O4 in zero magnetic ﬁeld. 3)

Figure 1: Magnetic ﬁeld dependence of the magnetic
Bragg intensities at (1/2, 1/2, 1/2), (1/2, 1/2, 3/2)and (1, 1, 1).

References
1) S. Diaz et al.: Phys. Rev. B 74, 092404 (2006).
2) T. Hoshi et al.: J. Mag. Mag. Mater. 310, e448(2007).
3) M. Matsuda et al., Europhys. Lett. 82,37006 (2008).

分野：中性子散乱（磁性）- 82 -

JAEA-Review 2013-039

1-2-11High-Pressure Neutron Diﬀraction Study of Magnetic Properties in DyB2 C2
H. Yamauchi and T. Osakabe
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

原子炉：JRR-3

装置：TAS-1(2G)30(a)
TN ( neutron, AFM 1 0 0 )
TN ( ref. 2) )TQ ( ref. 2) )TN , TQ (K)

25

20

15

DyB2C2Magnetic moment (μΒ/Dy)

The tetragonal DyB2 C2 shows an antiferroquadrupolar (AFQ) order below TQ = 24.7 K
in zero magnetic ﬁeld1) . Below TN = 15.3 K
the antiferromagnetic (AFM) order competitively coexists with the AFQ order. The
magnetic structure in the coexistent phase isdescribed by k1 = (1, 0, 0) and k2 = (0, 1, 1/2)
to give the basic 90◦ structure along the caxis, plus k3 = (0, 0, 0) and k4 = (0, 0, 1/2) togive the additional slight canting of magnetic
moments in the c-plane. The situation withthe variation of DyB2 C2 magnetic properties
under pressure is not so clear as that with
ambient pressure properties. There is only
one published report where the electrical resistivity studies were carried out on application of hydrostatic pressure up to 3.1 GPa2) .
We performed the neutron diﬀraction experiments under high pressures up to 8.8 GPa ona single crystal DyB2 C2 in order to investigate the P – T phase diagram and magnetic
structure under pressure.
The single crystal of Dy11 B2 C2 was prepared by the Czochralski method with a tetraarc furnace. The sample was cut and shaped
in a rectangle of 0.7 × 0.7 × 0.2 mm3 . We
succeed in experiments using an opposed pairof large anvils, named “ hybrid-anvil cell ”3) .
The measurements were carried out in thea∗ - a∗ reciprocal lattice plane with a neutron
wavelength of 2.444 Å. All the collimators and
PG ﬁlter were taken away to intensify the possible neutron beam ﬂux.
Figure 1-(a) shows the pressure dependenceof TN in DyB2 C2 . The transition temperatures are determined from the temperaturedependence of the peak intensity of AFM 1 0 0
reﬂection under pressure. The results of ref. 2)
are concurrently shown for comparison in theﬁgure. The TN increases linearly with pressure up to ∼ 6 GPa and seems to decrease
above ∼ 7 GPa. On the other hand, the TQ
decreases with increasing pressure and seems

10
6

(b)
9K

5

k1 = (1, 0, 0)

4
3
2

k3 = (0, 0, 0)

1
0

2

4

6

8

10

12

14

Pressure (GPa)Figure 1: The pressure dependence of (a) TN , TQ and(b) k1 , k3 components of magnetic structure at ∼ 9 K
in DyB2 C2 . Lines are guide for eyes.

to merge with TN at ∼ 7 GPa. Contrary to
the pressure dependence of TN , it is mysterious that the k1 components of magnetic
structure is suppressed by pressure as shownin Fig. 1-(b), since the AFM order describedby the wave vector of (1, 0, 0), which is observed in most of the RB2 C2 system, are considered to reﬂect the basic magnetic interactions in DyB2 C2 . It is, therefore, necessary
to measure k2 components which reﬂect theexistence of the competitive AFQ interactions
and to consider the eﬀects of the frustration
between the AFQ and AFM interactions.
References
1) H. Yamauchi et al.: J. Phys. Soc. Jpn., 68, 2057
(1999).
2) M. Kosaka et al.: “ Spring Meeting of Phys. Soc.
Jpn.”, 22pZF-5 (March, 2000).
3) T. Osakabe et al.: J. Magn. Magn. Mater. 310,
2725 (2007).

分野：中性子散乱（磁性）- 83 -

JAEA-Review 2013-039

1-2-12
Nematic-to-Smectic Transition of Magnetic Texture in Conical State
M. Takeda1,2 , Y. Endoh1,3 , K. Kakurai1 , Y. Onose4 , J. Suzuki2 and Y. Tokura4,5
Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195, Japan
2
J-PARC Center, Tokai, Ibaraki 319-1195, Japan
3
International Institute for Advanced Studies, Kizugawa, Kyoto 619-0225, Japan
4
Department of Applied Physics, University of Tokyo, Tokyo 113-8656, Japan& ERATO Multiferroics Project, JST, c/o University of Tokyo, Tokyo 113-8656, Japan
5
Cross-Correlated Materials Research Group, ASI, RIKEN, Wako 351-0198, Japan

Measurements of SANS have been performed using SANS-J-II. A single crystal of
Fe0.7 Co0.3 Si (∼0.1 cm3 ) grown by the ﬂoatingzone method4) . The helical spin modulation ischanged to the commensurate ferromagnetic
order through a conical spin state by applying external magnetic ﬁeld. The external ﬁeld
was applied up to 0.2 T where the spiral phase
disappears. Temperature was controlled between 4 and 60 K.

0.3

装置：SANS-J(C3-2)

0.3

4.5 K, 0.0T

0.1
-1

qy (nm )-1

qy (nm )0.075T

0.2

0.1
0.0

[100]

-0.1
-0.2

0.0
-0.1
-0.2

B

-0.3

-0.3
-0.3

-0.2

-0.1

0.3

0.0

-1

qx (nm )

0.1

0.2

-0.3

0.3

-0.2

0.3

0.125T

0.2

-0.1

0.0

-1

qx (nm )

0.1

0.2

0.3

0.20T

0.2

0.1

0.1
-1

0.0
-0.1

0.0
-0.1

-0.2

-0.2

-0.3
-0.3

-0.2

-0.1

0.0

-1

qx (nm )

0.1

0.2

0.3

-0.3
-0.3

-0.2

-0.1

0.0

-1

qx (nm )

0.1

0.2

0.3

Figure 1: Magnetic ﬁeld dependence of the colorcoded scattering proﬁles. The external magnetic ﬁeld
was increased from μ0 H = 0 to 0.2 T at 4.5 K.

References
1) M. Lee, Y. Onose, Y. Tokura, and N. P. Ong:
Phys. Rev. B 75 (2007) 172403.
2) C. Pﬂeiderer, G. J. McMullan, S. R. Jurian, andG. G. Lonzarich: Phys. Rev. B 55 (1997) 8330.
3) G. L. Squires: Introduction to the Theory of Thermal Neutron Scattering (Dover, New York, 1996)
p. 186.
4) Y. Onose, N. Takeshita, C. Terakura, H. Takagi,
and Y. Tokura: Phys. Rev. B 72 (2005) 22443.
5) M. Takeda, Y. Endoh, K. Kakurai, Y. Onose, J.
Suzuki, and Y. Tokura: J. Phys. Soc. Jpn. inpress.

Figure 1 shows magnetic ﬁeld dependenceof the color-coded scattering proﬁles on acommon logarithmic scale at 4.5 K. The representative patterns show clear changes inscattering proﬁles, i.e., circular → ellipsoidal→ crescent → double dots, with ﬁeld application along the [100] axis. This indicates that
原子炉：JRR-3

[010]

0.2

qy (nm )The microscopic structure of spin moments,
particularly the complex structures of an antiferromagnet with a long-range spin modulation cannot be exclusively determined without neutron magnetic scattering study3) . In
this study, we found unique neutron diﬀraction patterns manifesting the existence of acomplex magnetic texture in the bulk material of Fe0.7 Co0.3 Si.

a phase transition of magnetic texture occurs.
Throughout this phase transition, the change
in the diﬀraction patterns is very similar tothat observed in the nematic and smectic
phase transitions of liquid crystals. The details of this study will be reported elsewhere5) .

-1

Unconventional magnetic properties suchas the anomalous Hall eﬀect1) and quantum phase transition under high pressure2)
in the helimagnetic phase of the MnSi family
have currently attracted considerable interest. The non-centrosymmetric crystal structure of a simple cubic lattice (P21 3 , or B20type) is inherent in the MnSi family including
Fe1−x Cox Si. This low symmetry of the crystal structure hosts a long-range helimagnetic
spiral spin modulation via the DzyalosinskyMoriya (DM) interaction.

qy (nm )1

分野：中性子散乱（磁性）- 84 -

JAEA-Review 2013-039

1-2-13
Anisotropic Spin Freezing in Lightly-Doped La2−x Srx CuO4
M. Matsuda, M. Fujita1 , M. Takeda, K. Kakurai and K. Yamada1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Institute for Materials Research, Tohoku University, Sendai 980-8577

The interplay between magnetism and conductivity is crucial to understand the mechanism of superconductivity in high-Tc cuprate
superconductors.
The mother compound
La2 CuO4 shows a Néel ordering below ∼320
K. When hole carriers are doped, the magnetic ordering is quickly destroyed at x∼0.02.
The short-ranged magnetic correlations remain even above x∼0.02. Extensive neutronscattering studies have shown that the spincorrelations of the short-ranged magnetic
phase are incommensurate. Furthermore,
the static spin modulation in La2−x Srx CuO4
changes from being diagonal to parallel atx∼0.055, coincident with the insulator-tosuperconductor transition 1, 2) . This shows
an intimate relation between magnetism andconductivity. One possibility to explain the
diagonal incommensurate spin correlations is
the stripe model. On the other hand, the diagonal incommensurate spin correlations canbe explained using the spiral model, originating from magnetic frustration caused by the
localized hole spins. In order to understandthe nature of the incommensurate spin correlations in this region, it is important to clarify
the magnetic anisotropy (Heisenberg, XY, or
Ising) and determine the spin Hamiltonian.
Inelastic neutron scattering experiments
were performed to observe the zone center gap
originating from the magnetic anisotropy inthe diagonal incommensurate phase 3) . Since
the magnetic excitations become broadened,
it is not clear whether the gap disappears or
the magnetic excitations are just smeared out
so that the gap is diﬃcult to be identiﬁed.
Polarized neutron scattering is an important tool to clarify the magnetic anisotropy
in the magnetic materials.
Using threedimensional (3D) polarization analysis 4) ,we clariﬁed the magnetic anisotropy in
La1.982 Sr0.018 CuO4 and determined that the
原子炉：JRR-3

装置：TAS-1(2G)

XY model is the most suitable model to describe the low energy spin ﬂuctuations.
Unpolarized neutron scattering measurements were performed on TAS-2. The ﬁxed
initial neutron energy was 14.7 meV with an
instrumental energy resolution of ΔE ∼ 1.6
meV. Polarized neutron scattering measurements were performed using CRYOgenic Polarization Analysis Device (CRYOPAD) installed on TAS-15) . Heusler alloy (111) crystals were used as monochromator and analyzer. A ﬂipping ratio of ∼30 was measured
at the nuclear (200) reﬂection, corresponding
to 93% polarization of the beam. The incident neutron energy was ﬁxed at Ei =14.7
meV with an instrumental energy resolutionof ΔE ∼ 1.7 meV.
It
waspreviously
reportedthat
La1.982 Sr0.018 CuO4 exhibits a Néel orderingand spin-glass behavior at low temperatures
6) . The spin-glass phase shows short-ranged
antiferromagnetic ordering with diagonal
incommensurate correlations. Since the magnetic correlation perpendicular to the CuO2
plane is ﬁnite, a modulation of scattering
intensity along L direction is observed, as
shown in Fig. 1. The correlation length along
the c axis was estimated to be 11 Å6) , whichalmost corresponds to c. The signal contains
quasi-elastic component with ﬁnite energy
ﬂuctuations (|E| < ΔE). It is noted that theincommensurate magnetic peaks are not in
the scattering plane, as shown in Fig. 1. The
vertically elongated instrumental resolution
integrates the two peaks eﬀectively. Therealso exist magnetic Bragg peaks at thecommensurate positions (1, 0, even), which
originate from the Néel ordering. However,since the peaks are very sharp, the broad
signal shown in Fig. 1 purely comes from thespin-glass phase.
In the porlarization analysis we measured

分野：中性子散乱（磁性）- 85 -

JAEA-Review 2013-039

Table 2: Polarization matrix elements Pif observed at(1, 0, 3.9).

i\f
x
y
z

Figure 1:
Magnetic elastic scattering in
La1.982 Sr0.018 CuO4 at (1, 0, L) at T =4.5 K,
measured with unpolarized neutrons. The background signal measured at 60 K was subtracted.
The arrows show the positions where the neutron
polarization analysis was performed. The inset shows
the conﬁguration of incommensurate magnetic Bragg
peaks in the (H0L) scattering plane. The verticallyelongated instrumental resolution, shown by a shaded
ellipsoid, eﬀectively integrates the two magnetic
peaks (open circles), which are located above andbelow the scattering plane.
Table 1: Polarization matrix elements Pif observed at(1, 0, 0.1).

i\f
x
y
z

x
-0.9(1)0.11(9)0.04(8)y0.09(8)-0.7(1)-0.05(8)z0.03(7)0.00(7)0.7(1)

two diﬀuse magnetic peaks at (1, 0, 0.1) and(1, 0, 3.9). The neutrons observe only thespin component perpendicular to Q. Therefore, at (1, 0, 0.1), where Q is almost along
the a axis, the magnetic anisotropy in the bc
plane can be observed. On the other hand,at (1, 0, 3.9), where Q is ∼60◦ tilted fromthe ab plane, the magnetic anisotropy mostly
in the ab plane can be observed. Combining
these two results, it is possible to estimate themagnetic anisotropy in the spin-glass phase.
Table 1 shows the results of 3D polarization
analysis at (1, 0, 0.1) in the spin-glass phaseof La1.982 Sr0.018 CuO4 . The polarization matrix has nine elements Pif with i, f =x, y, andz, where i and f represent ”initial” and ”ﬁnal”, respectively. Since the signal is purely
magnetic in origin, Pxx corresponds to initial
beam polarization. It was observed that allx-0.90(8)0.04(4)0.01(4)y0.00(4)-0.25(3)-0.01(4)z0.03(4)0.05(4)0.32(6)the non-diagonal terms are negligibly small.
Pyx and Pzx are chiral terms that should become ﬁnite in the presence of helicity in themagnetic structure. In the present experiment, the chiral terms should become zero inprinciple even when the structure has helicity, since two incommensurate peaks, which
are related with positive and negative helicities, are integrated so that two contributions
are cancelled out. We plan to perform polarized neutron scattering experiments to clarify
the helicity in the future. From the polarization components Pyy , Pyz , Pzy and Pzz , it
was estimated that the ratio between the spincomponents along the b axis (Sb ) and along
the a axis (Sa ) is Sb /Sa ∼1.2.
Table 2 shows the results of 3D polarization analysis at (1, 0, 3.9). The polarization
components are similar to those at (1, 0, 0.1)
except Pyy and Pzz . From these values, it
was estimated that the ratio between Sb andthe spin component along the c axis (Sc ) is
Sc /Sb ∼0.15.
From the above two results, we conclude
that Sa : Sb : Sc ∼0.8 : 1.0 : 0.15. It was
found that the low energy spin ﬂuctuations(|E|<1.7 meV) have the XY anisotropy in
La1.982 Sr0.018 CuO4 although there also exists
a small Ising anisotropy along the b axis in theab plane. This reminds us that pure La2 CuO4
shows a Néel ordering with an easy axis along
the b axis.
References- 86 -

1) S. Wakimoto et al., Phys. Rev. B 60, R769 (1999).
2) M. Fujita et al., Phys. Rev. B 65, 064505 (2002).
3) M. Matsuda et al., Phys. Rev. B 62, 9148 (2000).
4) F. Tasset, Physica B 156-157, 627 (1989).
5) M. Takeda et al., Physica B 356, 136 (2005).
6) M. Matsuda et al., Phys. Rev. B 65, 134515 (2002).

1-2-13

JAEA-Review 2013-039

1-2-14Magnetic Structural Analysis of Magnetic Multilayers for Read Sensor Heads
by Polarized Neutron Reﬂectometry
M. Takeda1,2 , D. Yamazaki1,2 and T. Hirano3
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195, Japan
2
J-PARC Center, Tokai, Ibaraki 319-1195, Japan3
Hitachi Research Laboratory, Hitachi Ltd., Hitachi, Ibaraki, Japan

A read sensor head is one of key elements toachieve higher recording density of hard disk
drives (HDDs). The read sensor head of HDD
consists of several ferromagnetic, antiferromagnetic, and noble metal layers. The characterization of the magnetic interfacial structure in these magnetic multilayers is indispensable for producing the high-performanceand high-reliability read sensor heads, because the device properties strongly dependon the structure.
Neutron reﬂectometry is a powerful andnondestructive technique to investigate theinternal layered structures, and gives us theinformation on the depth proﬁle of magnetization vector of the magnetic multilayers in
the reﬂection plane. When polarized neutron
is used, the sensitivity to the magnetization ismuch enhanced1) . Therefore, polarized neutron reﬂectometry is an unrivaled way to analyze the internal magnetic structure in magnetic multilayers.
Figure 1 shows a typical example ofthe investigation of the magnetic multilayers for the read sensor heads using a
H=1.8 kOe

CoFe

M

new neutron reﬂectometer, SUIREN, installed at the C2-2 cold neutron beam portof the beam hall in JRR-3, of JAEA2) .
Structures of the samples are describedas Si(substrate)/Ta(5 nm)/Ru(5 nm)/MnIr(xnm)/CoFe(2 nm)/Cu(1nm)/Ru(2 nm) (x =3.0 (sample A) and 5.0 (sample B)). Exchange
bias between the CoFe and MnIr layers ofsample B is larger than that of sample A.
The reﬂectivity was measured under an external magnetic ﬁeld of 1.8 kOe perpendicular
to the magnetized direction. An intermediate layer at the interface between the CoFe
and MnIr layers was found only in sample B.
This intermediate layer may be a key to elucidate the mechanism of the exchange bias effect. The details of this experiment will bereported elsewhere.
References
1) G. P. Felcher, R. O. Hilleke, R. K. Crawford, J.
Haumann, R. Kleb, and G. Ostrowski, Rev. Sci.
Instrum. 58, 609 (1986).
2) D. Yamazaki, M. Takeda, I. Tamura, R. Maruyama,
A. Moriai, M. Hino, K. Soyama, Physica B 404,
2557 (2009).

CoFe/MnIr
interfaceM =1.63μB
=44゜

(a)

M

=0.5μB=63゜(b)Figure 1: Diﬀerence of the polarized neutron reﬂectivity curves with a change of thickness of the MnIr layer; (a)3 nm and (b) 5 nm. An external magnetic ﬁeld of 1.8 kOe was applied perpendicular to the magnetized axis.

原子炉：JRR-3

装置：SUIREN(C2-2)

分野：中性子散乱（磁性）- 87 -

JAEA-Review 2013-039

1-2-15Acquirement of a Guiding Principle Towards the Dy-free or Dy-lessHigh Performance Nd-Fe-B Sintered Magnets
by Investigation of the Origin of the Coercivity with Interfacial Structural
Analysis
M. Takeda1,2,4 , J. Suzuki2 , D. Yamaguchi3 , T. Akiya4 ,H. Kato4,5 , Y. Une6 and M. Sagawa4,6
1

QuBS, Japan Atomic Energy Agency, Tokai-mura, Ibaraki, 319-1195, Japan
2
J-PARC Center, Tokai-mura, Ibaraki, 319-1195, Japan
3
ASRC, Japan Atomic Energy Agency, Tokai-mura, Ibaraki, 319-1195, Japan
4
New Industry Creation Hatchery Center, Tohoku Univ., Sendai, Miyagi, 980-8579, Japan
5
Depertment of Applied Mathematics and Physics, Yamagata University,
Yonezawa, Yamagata, 992-8510, Japan
6
Intermetallics Co., Ltd., Kyodaikatsura #303, 1-36 Goryo Ohara, Nishikyo-Ku,
Kyoto, 615-8245, Japan

Nd-Fe-B magnets are useful permanent
magnets utilized in many applications such as
motors, HDD and mobile phones. Recently,
they are used in motors of hybrid electric vehicles (HEV) which is one of the most promising
application of Nd-Fe-B magnets. As high heat
resistance and high coercivity are strongly required in HEVs, some amounts of Dy areadded to Nd-Fe-B magnets.
However, the natural abundance of Dy is
quite low and producing countries are limited.
Therefore, the development of Dy-free or Dyless Nd-Fe-B sintered magnets with high coercivity is strongly demanded. In order to enhance the coercivity, grain reﬁnement of microstructure in sintered magnets and the microstructural control at the interface between
Nd2 Fe14 B and Nd-rich phases are important.
We performed small-angle neutron scattering (SANS) measurements of the Nd-Fe-B sintered magnets using unpolarized and polarized neutrons to get information on the averaged internal inhomogeneous structure of
Nd-Fe-B sintered magnets including the interfacial structures which is the key parameterto achieve the high-coercivity Dy-free Nd-FeB sintered magnet. The SANS experiments
were performed using PNO and SANS-J-II.
Intensity distributions of SANS from the
Nd-Fe-B sintered magnets on a 2-dimensional
position-sensitive detector of SANS-J-II (intensity maps) were sensitive to the sintering and annealing condition of the samples,as shown in FIg. 1. The patterns were also
原子炉：JRR-3

装置：SANS-J(C3-2)

120(a) 1000C 3 μ m

120

100

100

80

80

60

60

40

40

20

c-axis0(b) 960C 1.2 μ m

20
0

0

20

40

60

80

100

120

0

20

40

60

80

100

120

Figure 1: Color-coded intensity maps of Nd-Fe-B sintered magnets with diﬀerent sintering process; (a) 3
μm powders sintered at 1000 ◦ C, and (b) 1.2 μm powders sintered at 960 ◦ C.

drastically changed by changing the temperature and applying magnetic ﬁeld during measurements. These observations indicate that
the SANS measurement is a promising tool
to investigate the correlation between the coercivity and the internal structure of Nd-FeB sintered magnets. We are going to extend
this work to elucidate the high-magnetic-ﬁeld
annealing phenomenon1) , which improves thecoercivity, in the next ﬁscal year.
This work was supported by New Energy
and Industrial Technology Development Organization (NEDO), Grant-in-Aid for ”Development of technology for reducing dysprosium usage in a 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.

PNO(3G)- 88 -

分野：中性子散乱（磁性）JAEA-Review 2013-039

1-2-16
Polarized Neutron Diﬀraction Study of Magnetic Chirality in Multiferroic
Compound TmMn2 O5
S. Wakimoto, H. Kimura1 , M. Fukunaga1 , M. Takeda, K. Kakurai, and Y. Noda1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577

Multiferroic materials RMn2 O5 show antiferromagnetic order and ferroelectricity concomitantly at low temperatures with strong
coupling. To date, two models are suggested
as an origin of the magnetic driven ferroelectricy in this system. One suggests P ∝Si ×Sj 2) while the other suggests P ∝ Si ·Sj . 3)
Previously we have shown that the magnetic
chirality is proportional to the FE polarization for materials with R =Ho and Er, consistent with the S × S model. 4) Recenltly it isfound that TmMn2 O5 shows polarization ﬂop
transition at 4 K from P//b to P//a as temperature decreases. 5) Since the S × S model
requires one to one correspondence between
the chiral plane and the polarization, a studyof the magnetic chirality at the ﬂop transition
should give another test of the model.
Polarized neutron diﬀraction study was carried out at TAS-1 spectrometer with PG
monochromator and Huesler analyzer. In thiscase, diﬀracted neutron cross-sections with
diﬀerent polarizations σ+ and σ− , i.e. spin up

and down, correspond to the diﬀerent chirality. During the measurement, external electric ﬁeld has been applied to the a-axis.
Figure 1 shows the cross-sections σ+ andσ− measured near (1.5, 0, 0.25). At this Q,
one can observe the magnetic chirality in thebc-plane which gives P//b on the basis of the
S × S model. As shown in Fig. 1, the magnetic chirality which can be characterized by
the diﬀerence in σ+ and σ− disappears in the
P//a phase. This proves that the polarization ﬂop transition is indeed accompanied by
the change of the chiral plane consistent with
the S × S model.
References
1) T. Kimura et al., Nature 426, 55 (2003).
2) H. Katsura, N. Nagaosa, and A. V. Balatsky, Phys.
Rev. Lett.95, 057205 (2004).
3) L. C. Chapon et al., Phys. Rev. Lett.96, 097601(2006).
4) S. Wakimoto et al., doi:10.1016/j.physb.2009.06.012.
5) M. Fukunaga et al., J. Phys. Soc. Jpn. 77, 094711(2008).

TmMn 2O530

σ-(H, 0, 0.284)
σ−

σ+

20
6K
P // b

10
0
1.3

Q

1.4

1.5
1.6
H (r.l.u.)

3.8 K
P // a

1.7

1.4

σ+
Q

1.5
1.6
H (r.l.u.)

1.7

Figure 1: Polarized neutron diﬀraction data at 6 K and 3.8 K near (1.5, 0, 0.25). Cross-sections σ+ and σ−correspond to the diﬀerent chiralities as shown in the inset.

原子炉：JRR-3

装置：TAS-1(2G)

分野：中性子散乱（磁性）- 89 -

JAEA-Review 2013-039

1-2-17
A Small-Angle Polarized Neutron Scattering Experiment of Spherical
Fe16 N2 Nano-Particles for High Density Magnetic Recording Tape
H. Hagiya1,3 , T. Oku1 , H. Kira1 , T. Shinohara1 , J. Suzuki1 ,Y. Tamai2,3 , M. Takeda2 ,K. Kakurai2 , Y. Sasaki4 , M. Kishimoto4 , M. Yokoyama3 , Y. Nishihara3
Japan Proton Accelerator Research Complex center, JAEA, Tokai, Ibaraki 319-1195
2
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
3
Department of Science, Ibaraki University, Mito, Ibaraki 310-8512
4
Hitachi Maxell, Ltd., Koizumi, Oyamazaki-Cho, Otokuni-Gun, Kyoto 618-8525

原子炉：JRR-3

装置：SANS-J(C3-2)

that the experimental data were reproduced
better with model 2 than model 1 for the 2
samples. According to the sample preparation method 2) , model 2 is considered more
appropriate for the samples. Therefore, we
evaluated the surface layer thicknesses of thesamples based on the analysis with model 2,
and the non-magnetic surfactant layer thicknesses were determined to be 3.4 nm and 3.6
nm for sample M2 and M6, respectively.
1000(a) model 1
100

Intensity [a.u.]

Fe16 N2 exhibits a large magnetic momentand large crystalline anisotropy. Hence, theindustrial researchers have developed magnetically stable spherical Fe16 N2 nano-particles
for high density magnetic recording tape. The
surface of the particles is coated with a nonmagnetic layer to prevent oxidization andsintering. The optimization of the surfactant layer thickness is important to maximize
recording performance of the magnetic tape.
Then, in this study, we performed polarized
small-angle neutron scattering (SANS) experiments to evaluate their non-magnetic surfactant layer thickness quantitatively. According
to the previous study 1) , it was suggested thatscattering intensity proﬁles which reﬂect the
information of surface layer thickness would
appear intensively in the range q ≥∼ 1 nm−1 .
Thus, we performed SANS experiments in therange of 0.15 nm−1 < q < 2 nm−1 about
2 samples (M2 and M6) of Fe16 N2 nanoparticles with diﬀerent surface layer thicknesses. We applied a magnetic ﬁeld of 1 T
to the samples and measured SANS intensities of I + and I − of the cases that the spinpolarity of incident neutrons is positive andnegative, respectively. Fig. 1 shows the scat+−tering intensities I⊥
and I⊥
along the direction perpendicular to the applied magnetic
ﬁeld direction. Here, we analyzed the datawith 2 core-shell models in which we madeassumptions as follows: 1) In model 1, thethickness of the nonmagnetic surfactant layer
is independent of the particle diameter. 2) In
model 2, the ratio of the volumes of the magnetic core and nonmagnetic surfactant layer
regions is constant. The ﬁtting results withthe models are shown in Fig. 1. It was found

10

M2
1

Exp

Fit

2

3

+

I
I

0.1

6 7

0.1

4 5 6 71

2

-1q [nm ]
1000(b) model 2
100

Intensity [a.u.]

1

10
1

M2

0.1

Exp

Fit

2

3

+

I
I

0.01
6 7

0.1

4 5 6 71

2

-1q [nm ]

Figure 1: I vs. q.

References
1) T. Oku, et al. :“Physica B” (2009) in press.
2) Y. SASAKI, et al. :“IEEE Trans. Mag.” 41 (10)pp. 3241-3243 (2005).

分野：中性子散乱（磁性）- 90 -

JAEA-Review 2013-039

1-2-18Magnetic Structure in the Shastry-Sutherland Lattice TmB 4
Iga F.(a), Shigekawa A.(a), Michimura S.(a), Takabatake T.(a), Yoshii S.(b), YamamotoT.(b), Hagiwara M.(b), Kindo K. (c), Ohoyama K.(d)(a) ADSM, Hiroshima Univ., (b) KYOKUGEN, Osaka Univ., (c) cInstitute for Solid State
Physics, Univ. of Tokyo, (d) IMR, Tohoku Univ.
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) [1]
where nearest-neighboring dimers geometrically frustrated.
The previous study of TmB4 indicates
an antiferromagnetic order at 11.7 K by
the measurements of temperature dependences of electrical resistivity and magnetic susceptibility [2]. From our recent
experimental results, we have found that
TmB4 exhibits three phase transitions at
TN1=11.7K, T*=11K and TN2=10K [3]. The
phase transitions at TN1 and TN2 were already reported by Fisk et al [2]. In order toclarify these ordering vectors in these magnetic phases, we have performed neutron
diffraction experiment on Tm11B4.
First, high-quality single crystal TmB4
was grown by ﬂoating zone method using a four-xenon lamps image furnace.
Next, these crystals were crushed to powder. The neutron powder diffraction experiment was performed on the powder diffractometer for high efﬁciency andhigh resolution measurements, HERMES.
Measured temperatures were set at 3K(antiferro-magnetic phase, IV), 10.7K (unknown phase, III), 11.7K (unknown phase,II) and 20K (paramagnetic phase, I).
Figure 1 shows the powder pattern for
the four phases of TmB4. The pattern at
20 K was used for the nuclear scattering
standard. Phase IV shows a simple antiferromagnetic pattern with a propagation
vector of k4=(1, 0, 0). This is consistent
with the previous report [2]. The Phase III
has been assigned with propagation vector
k4 and an additional long period modula-tion vector k3=(0.13, 0, 0). Furthermore, thephase II was also indexed with the k4 andk2=(0.012, 0.012, 0) and k2=(0.036, 0.012, 0).
However, we have not yet succeeded in obtaining complete ﬁtting parameter.
Magnetization process M(B//c) in TmB4
shows 1/8 and 1/2 plateaus at 1.7-1.4 T and
2-3 T, respectively. These characteristic behavior may be originated from geometricfrustration in not only magnetic dipole interactions but also electric multipole interactions.
References[1] B. S. Shastry and B. Sutherland, Physica
B & C 108B (1981), p. 1069.
[2] Z. Fisk et al., Solid State Commun. 39(1981), p. 1189.
[3] F. Iga et al., J. Magn. Magn. Mater. (2007)
in press.

Fig. 1. Fig. 1 Neutron powder diffraction patterns
for the four phases of TmB4. The bottom shows asimulation in the paramagnetic state.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 225- 91 -

JAEA-Review 2013-039

1-2-19Successive metamagnetic behavior in an easy-plane type antiferromagnet
ErNi2Ge2
Y. Tabata(A), M. Okue(A), H. Nakamura(A), N. Matsuura(B)(A) Graduate School of Engineering, Kyoto University, (B) ISSP, University of Tokyo

On the othre hand, a colinear sinusoidal
modulated magnetic structure of ErNi2Ge2
was reported by Andre et al. [2], where
the Er magnetic moment forms an angle
64 degree with the c-axis. In their model,
the c-axis component of the Er magnetic
moment is about half the size of the cplane component, contradicting the resultsof our magnetization measurements mentioned above. In order to determine the direction of Er magnetic moment in the antiferromagnetic state, we performed polarized neutron scattering experiments by using a single crystalline sample on the tripleaxis spectrometer 5G installed at JRR-3M
reactor.

ﬂip (NSF) magnetic scattering proﬁles witha scattering vector K = (2,0,0.75) in the condition of the polarization vector of neutron
P being perpendicular to the scattering vector. In this experimental condition, the direction of P or K is almost parallel to thec- or the a-axis respectively, and hence, theb- or the c-axis component contributes the
SF or the NSF scattering respectively. As
shown in Fig. 1, the NSF scattering is almost absent, indicating the c-axis component is almost 0. Hence, we have concluded
that ErNi2Ge2 is the easy-plane type antiferromagnet, as expected from the magnetization measurements.
[1] T. Inami et al., cond-mat/0709.0977.
[2] G .Andre et al., J. Alloys and Comp. 224,
253 (1995).

400
Intensity (counts/300sec)

A rare earth intermetallic compound
ErNi2Ge2 with a tetragonal ThCr2Si2-type
structure is a long-period antiferromagnet
with TN =3.0K and magnetic wave vector
km=(0,0,0.75). Our recent magnetization
measurements by using single crystalline
samples and crystalline-electric-ﬁeld (CEF)
analysis indicate that ErNi2Ge2 is aneasy-plane type magnetic anisotropy,
where the c-plane is a magnetic easy-plane.
Interestingly, a successive metamagnetic
behavior has been found in a magnetization process along the magnetic hard-axis,
c-axis. Such a metamagnetism along amagnetic hard-axis had also been found inanother easy-type anitferromagnet TbB4,
which has the Shastry-Surthreland lattice.
Recently, the multi-step metamagnetictransition in TbB4 had been explained
based on a model with a XY-type groundspin state and an Ising-type exited spinstate[1]. Now we are trying to understandthe metamagnetism in ErNi2Ge2 based ona similar model.

350
300

ErNi2Ge2
P

K, T=1.5K

SF
NSF

250
200
150
100
50
0
-50

0.68 0.7 0.72 0.74 0.76 0.78 0.8 0.82
L in (2,0,L) (r.l.u.)

Fig. 1. Magentic scattering proﬁle of polarized neutron at the magnetic wave vector K = (2,0,0.75) in thecondition of the polarization vector P being perpendicular to K. Closed and oped circles denote the SFand the NSF-scattering proﬁles respectively.

Figure 1 shows spin-ﬂip (SF) and non-spinActivity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 602- 92 -

JAEA-Review 2013-039

1-2-20Anisotropic magnetic diﬀuse scattering in an easy-plane type antiferromagnet
ErNi2Ge2
Y. Tabata, H. Taguchi, K. Matsuda, H. Nakamura
Graduate School of Engineering, Kyoto University

Intensity (arb. units)

10

4

10

3

10

2

10

1

10

0

10

4

10

3

10

2

ExperimentGaus.+M.Lor.
Modified Lor.
Gaussian

ErNi2Ge2
T=1.45K
q//[1,0,0]Cκ2θ
2θ
[1+(q/κ) ]θ=1.34

resolution limit

ExperimentGaus.+M.Lor.
Modified Lor.
Gaussian

ErNi2Ge2
T=1.45K
q//[1,1,0]Cκ2θ
2θ
[1+(q/κ) ]θ=1.34

resolution limit

101
100
104

Intensity (arb. units)

Figure 1 shows magnetic scattering proﬁles along the [1,0,0]-, the [1,1,0]- and the[0,0,1]-direction with the scattering vector Km = (0,0,3.25). The proﬁles along the[1,0,0]- and the [1,1,0]-directions contains awidespread diffuse-scattering component,
while the proﬁle along the [0,0,1]-direction
has only a sharp Gaussian component. This
result indicates that the long-range andthe short-range orders coexist in the antiferromagnetic region and the short-rangeorder is quite anisotropic. The correlation
length of the short-range order along the caxis is enough long that the peak proﬁle iswithin the resolution limit, suggesting theshort-range order consists of 1-dimensional
long-range helices along the c-axis. The
diffuse-scattering component in the c-plane
is better ﬁt by a modiﬁed Lorentzian withan anomalous exponent theta = 1.34, theform is written in Fig.1, than by a simple
Lorentzain. The physical meaning of theshift of theta away from 1 is unclear.

Intensity (arb. units)

A rare earth intermetallic compound
ErNi2Ge2 with a tetragonal ThCr2Si2-type
structure is a long-period antiferromagnet
with TN =3.0K and magnetic wave vector
km=(0,0,0.75). Our recent magnetization
measurements by using single crystalline
samples and crystalline-electric-ﬁeld (CEF)
analysis indicate that ErNi2Ge2 is an easyplane type magnetic anisotropy, where thec-plane is a magnetic easy-plane. Absenceof the third harmonic scattering and weakanisotropy in the c-plane strongly suggest
a helical magnetic order in this compound.
We have found an anomalous anisotropic
magnetic diffuse scattering in the magnetic
ordered phase.

10

3

10

2

10

1

Experiment
Gaussian

ErNi2Ge2
T=1.45K
q//[0,0,1]

resolution limit

100
í0.10

í0.05

0.00

0.05

0.10

í1

q=|KíKm| (Å )Fig. 1. Magnetic scattering proﬁles along (upper)
the [1,0,0]-, (middle) the [1,1,0]- and (lower) the[0,0,1]-direction with the scattering vector Km =(0,0,3.25).

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1-2-21

Magnetic structure of RCoSn (R=Tb, Ho and Er)
M.Kurisu, 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. We have shown that the crystalline electric ﬁeld effect plays an dominant role in their anisotropic magnetic behaivior. The temperature dependence ofmagnetic susceptibility is well explainedby the systematic variation of CEF parameters in TbTX compounds, TbNiSn, TbPdSn
and TbRhGe[1]. The easy axis of magnetization is the b-axis in these three compounds. Recently, we have found that it is
the a-axis in the isostructural compound
TbCoSn. The sign of second order CEF parameters of the compound have opposite
sign to other TbTX. In the present report,
we show preliminary experimental resultsof single crystal neutron diffraction on TbCoSn to examine its magnetic strucure.
Single-crystalline TbCoSn ingots weregrown by a Czochralski method using
a tetra-arc furnace in puriﬁed Ar atmosphere. The neutron diffraction measurements were performed at T1-1:HQR spectrometer installed at JRR-3M.
The SQUID magnetic susceptibility shows that antiferromagnetic ordering
takes place at TN = 20.2 K. Below TN,an anomaly indicative of another magnetic transition is observed at 4 K for thethree principal axes. The speciﬁc heat measurement also indicates the two magnetic
phases.
The magnetic reﬂection is observed in the
a*-b* reciprocal lattice plane below TN as
shown in Fig.1. The magnetic structure appears to be represented by the wave vector(0 0.25 0). The analysis is in progress.

References[1] Speciﬁc heat and high ﬁeld magnetization of a TbPdSn single crystal,
Yoshikazu Andoh, Do Thi Kim Anh, Hiroyuki Hoshino, Go Nakamoto, Makio
Kurisu, and Shinji Kawano, Physica B, 373(2006) 150-153.

Fig. 1. Magnetic and nuclear reﬂections in a*-b*
plane of TbCoSn.

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1-2-22

Relationship between Magnetic Structure and Ferroelectricity of LiCu2O2
Y. Yasui, K. Sato, Y. Kobayashi, T. Moyoshi, M. Sato and K. Kakurai*
Dept of Phys., Nagoya Univ., *JAEA
Materials with magnetic and ferroelectric
coexisting orders are called multiferroics
and attract much attention. The authorsgroup have found that LiVCuO4 is a multiferroic with quasi one-dimensional spin
S=1/2 chains of Cu2+ ions formed ofedge-sharing CuO4 square planes (called
CuO2 ribbon chains).1,2) For physical understandings of multiferroic nature, thiskind of spin 1/2 systems seem to be useful, because they do not have any complications arising from the multi-orbital effects,
and because quantum effects may also induce interesting phenomena.
LiCu2O2 with the CuO2 ribbon chains was
also reported to be multiferroic.3) However, because its correct magnetic structure
has not been reported, there are many unsolved problems on the relationship between observed ferroelectiric behaviors3)
and the magnetic structure:4,5) Concerning the magnetic structure, several groups
have reported their results obtained by justone of experimental methods, such as neutron scattering4) and 7Li-NMR,5) where we
can ﬁnd that any of the reported structure
cannot explain the other reported structures. Actually, the existence of the fourCuO2 ribbon chains in the unit cell makes
it difﬁcult to correctly determine the modulated magnetic structure of the present system. Here, we have determined the magnetic structure2, applying both the neutron
scattering and 7Li-NMR measurements for
single-crystal samples of LiCu2O2, and therelationship between the magnetic structure and dielectric or ferroelectric properties also studied here, has been discussed.
From the temperature (T) dependences ofthe speciﬁc heat and 7Li-NMR spectra, themagnetic transitions has been found at 24.5
K (≡ TN1) and 22.8 K (≡ TN2), where theferroelectric transition has also been observed at TN2. To determine the magnetic

structures of intermediate (TN2<T<TN1)
and low temperature (T <TN2) phases, theneutron scattering intensities were measured in the (h k 0) and (h k 2h) planes in
the reciprocal space at 12 K (<TN2), 23.3 K(TN2<T<TN1) and 50 K (>TN). To avoid
the large neutron absorption of Li, we used
7Li isotopes. At 12 K and 23.3 K, we observed magnetic superlattice reﬂections at
Q = (h, k ±δ, 0) and (h, k ±δ, 2h) (h= half-integer, k = integer and δ˜0.172).
The system has an incommensurate magnetic structure with the modulation vecalong
tor Q=?b* (or the pitch angle ˜62
the CuO2 ribbon chains). We have determined the magnetic structures of intermediate and low temperature phases to reproduce the neutron data and 7Li-NMR spectra simultaneously. At 23.3 K(in the intermediate phase), the system has been foundto have a collinear structure with the spins
along the c-axis and modulated in a sinusoidal way. It is consistent with the nonappearance of ferroelectricity in this phase.
The magnetic structure of the low temperature phase has also been determined. Basically, it is helical, and parameters to describe the detailed structure will be published soon.
We have found that the relation P ? Q ?
e3 holds (e3 is the helical axis) in zeromagnetic ﬁeld, which is consistent withthe existing theories. The existence of thecollinear phase above TN2, and the observed anisotropy of the amplitudes of themodulations, which form the helical structure may be related to a possible effect of
the quantum ﬂuctuation.
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)

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JAEA-Review 2013-039

057601.
[4] T. Masuda et al.: Phys. Rev. Lett. 92(2004) 177201.
[5] A.A. Gippius et al.: Phys. Rev. B 70
(2004) 020406.

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1-2-23Magnetic Properties of Honeycomb System Na2Co2TeO6
Y. Yasui, Y. Miura, T. Moyoshi, M. Sato and K. Kakurai*
Dept of Phys., Nagoya Univ., *JAEANa2Co2TeO6, has Co2TeO6 layers, consisting of edge-sharing CoO6- and SbO6octahedra with Na layers between them.
The Co2+ ions are considered to have highspin state S=3/2. For this system, polycrystalline samples of Na2Co2TeO6 wereprepared, and their magnetic susceptibility and speciﬁc heat were ﬁrst measured,
where clear anomalies due to the antiferromagnetic transition1) were found in thetemperature dependences of these quantities at TN=23.7 K. The magnetic susceptibility data have been analyzed using thehigh temperature expansion method, andthe ﬁrst-, second- and third-neighbor interactions J1, J2 and J3 among the spins are estimated to be 11.4 ± 0.5 K (Ferro), -4.1 ±0.1 K (AF) and 0.3 ± 0.1 K (Ferro), respectively. Based on the J1/J3-J2/J3 phase diagram of Heisenberg spin system proposedby Fouet et al.,2) the magnetic structure ofthis system is expected to be screw typeone. To see if the structure is actually foundin this system, neutron scattering measurements were carried out using the triple axis
spectrometer HQR (T1-1), where the double axis condition was adopted. At T=4
K, we observed the magnetic reﬂections
at commensurate Q-points. Figure shows
the T-dependence of the integrated intensity of 1 0 1 magnetic reﬂection. From theﬁgure, the magnetic ordering is found togrow with decreasing T below TN. By the
preliminary analyses of the neutron scattering data, the magnetic structure which
can reproduce the observed magnetic scattering intensities at 4 K is obtained (shown
schematically in the inset of the ﬁgure). The
details of the obtained structure at 4 K canbe described as follows. The collinear ordering of the Co2+ moments can be foundwith the moment direction parallel to thec-axis. In the honeycomb layer, the onedimensional zig-zag ferromagnetic chains

exist and these ferromagnetic chains orderantiferromagnetically. The discrepancy between the predicted and actual magnetic
structure of Na2Co2TeO6 seems to be originated from the anisotropy of the Co2+
spins with strong Ising anisotropy.
References[1] Y. Miura et al.: J. Phys. Soc. Jpn. 75 (2006)
084707.
[2] J.B. Fouet et al.: Eur. Phys. J. B 20 (2001)
241.

Fig. 1.

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1-2-24Magnetic structure of multiferroic DyMnO3 studied by polarized neutron
diﬀraction
D. Okuyama(A), H. Murakawa(B), K. Iwasa(C), H. Sagayama(D), Y. Kaneko(B), Y.
Taguchi(A), T. Arima(D), and Y. Tokura(A,B,E)(A)RIKEN-CMRG, (B)ERATO-MF, (C)Tohoku Univ., (D)Tohoku Univ.-IMRAM, (E) Univ. ofTokyo
Recently, perovskite manganites havebeen intensively studied from the view
points of multiferroics properties [1]. In
typical multiferroics material TbMnO3 and
DyMnO3 , polarization ﬂop phenomena areobserved under the magnetic ﬁeld [1]. Recent theoretical studies [2, 3] suggest thatthe cycloidal magnetic structure of Mn
ion plays an important role to the ferroelectric state. In Ref. [2], ferroelectric
polarization of multiferroics TbMnO3 and
DyMnO3 can be expressed by cross product between the magnetic propagation vector and magnetic chirality from cycloidal
structure as P=α k × (Si × S j ). On the basis of this theory, the origin of polarization
ﬂop phenomena from P//c to P//a canbe understood as being due to the magnetic structural phase transition from bccycloidal magnetic structure to ab-cycloidal
magnetic structure. For ensuring this theoretical prediction, the magnetic structure of
P//c phase at zero ﬁled and P//a phase
under hight magnetic ﬁelds should be clariﬁed. Therefore, we utilized polarized neutron diffraction method and tried to decide
the precise magnetic structure in both zeroand high magnetic ﬁelds.
As the target material, we chose
DyMnO3 , which shows the polarization ﬂop phenomenon at low magnetic
ﬁled (∼2 Tesla). Neutron diffraction experiments were performed on TOPAN
triple-axis spectrometer. Neutron beamwith an energy 80 meV was used. A
single crystal of DyMnO3 was mounted inlongitudinal magnetic ﬁled-type superconducting magnet (Endoh-magnet) so thatthe [1 0 0]-[0 0 1] direction on Pbnm setting
were parallel to the scattering plane.
First, we tried to measure the eight mag-netic reciprocal lattice points marked with
red circles in Fig. 1 with unpolarized neutron diffraction mode for charactering themagnetic properties at low temperature of
DyMnO3 . In Fig. 1, the peak proﬁles ofmagnetic reﬂections at (0 k 5), (0 k 6), (1 k
5), (1 k 6), (5 k 0), (6 k 0), (4 k 1), (5 k 1)
positions are shown. Black triangle, red triangle, and blue circle indicate the peak proﬁles at T=15 K, 8 K, and 6.5 K near the ferroelectric ordering temperature TC =18 K andthe magnetic ordering temperature of Dy
moment TN−Dy =6.5 K, respectively. In thedata at 8 K (6.5 K≤ T ≤18 K), only (0 0.38
5) and (4 0.38 1) reﬂections were observed,
in which the magnetic moment of Mn ion ismainly involved. In contrast, in the data at
3 K (T ≤6.5 K), additional (0 1/2 5) and (51/2 0) were observed. These experimental
results are consistent with the data of Ref.
[4].
In order to decide the magnetic structures of Mn moment at both zero and highmagnetic ﬁelds, we utilized polarized neutron diffraction method. For the limitation of the experimental conﬁguration, we
measured only (0 0.38 5) magnetic reﬂection. In this case, we can mainly observe
the magnetic reﬂection from a-axis (b-axis)
magnetic component at spin ﬂip (non-ﬁlp)
process, respectively. In Fig. 1, at 0.5 Tesla(near zero ﬁeld P//c phase), only the magnetic reﬂection from non-spin ﬂip process
was observed. This result strongly suggests the bc-cycloidal magnetic structure of
Mn moment, which is consistent with thedata of Ref. [4]. On the other hand, at 3.5
Tesla (P//a phase), the small magnetic reﬂections from both non-spin ﬂip and spin
ﬂip processes were observed with slightly
poor statistics. From this result, we con-

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JAEA-Review 2013-039

cluded that the ab-cycloidal magnetic structure of Mn moment is realized in P//aphase at high magnetic ﬁelds.
In summary, we determined roughly themagnetic structure of Mn moment of multiferroic DyMnO3 in both P//c phase at
low magnetic ﬁelds and P//a phase at highmagnetic ﬁelds. These magnetic structures
support the theoretical prediction that thepolarization ﬂop phenomenon is due to thechange of the cycloidal spin plane from bcplane to ab-plane.
[1] T. Kimura et. al.: Nature 426, 55(2003).; Phys. Rev. B 71, 224425 (2005). [2]
H. Katsura et. al.: Phys. Rev. Lett. 95,
057205 (2005). [3] M. Mochizuki et. al.: eprint available at arXiv:0811.4015. [4] O.
Prokhnenko et. al.: Phys. Rev. Lett. 98,
057206 (2007).

Fig. 1.

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1-2-25

Neutron Diﬀraction Studies on Dy7Rh3Dx
T. Tsutaoka(A), A. Tanaka(A), G. Nakamoto(B), M. Kurisu(B), Y. Andoh(C), R. Sato(D),S. M. Filipek(D)(A)Graduate School of Education, Hiroshima University, (B)Japan Advanced Institute of
Science and Technology, (C)Faculty of Regional Sciences, Tottori University, (D) Institute ofPhysical Chemistry, Polish Academy of Sciences
The 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; magnetic property of the Tb7Rh3 and Dy7Rh3changes from antiferromagnetic to ferromagnetic or ferrimagnetic and the electrical property changes from semimetallic tometallic by the hydrogenation[1]. In thisstudy, we have performed powder neutron diffraction measurements on the magnetic deuteride Dy7Rh3D28 to investigate
the magnetic structure. Hydrogenation of
R7Rh3 samples were carried out in thepressure up to 10 kbar at 25 and 100 degree Celsius in the high pressure apparatus [2]. 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 awave length of 1.82645(6) A.
Figure 1(a) shows the powder neutron
diffraction proﬁles of Dy7Rh3 at 3.5 K, 40
K and 70 K. A large (000)+ magnetic reﬂection was observed in the magneticallyordered states below TN = 59 K. Nuclear
peaks can be indexed by the Fe7Rh3 typestructure. Figure 1(b) shows the powder
neutron diffraction proﬁles of Dy7Rh3D28
at 4.5 K and 70 K. The (000)+ magnetic reﬂection was also observed in the duteride
Dy7Rh3D28. This result indicates that the
Dy7Rh3Dx also has the antiferromagnetic
interactions. From the past studies, since
R7Rh3 compounds tend to have helical orconical magnetic structures, Dy7Rh3 canhave the helical magnetic structure. For the
R7Rh3 deuterides, the conﬁguration of thehydrogen has not been determined. Thus
the study for the magnetic structure aswell as the hydrogen structure investigation for Dy7Rh3 and its hydrides is now
in progress.
References[1] R. Sato, T. Tsutaoka, S.M. Filipek, J. Alloys and Comp., 446-447 (2007) 610.
[2] B. Baranowski, S.M. Filipek, J. Alloys
and Comp., 404-406 (2005) 2.

Fig. 1. Fig.1 Neutron diffraction proﬁles for Dy7Rh3(a) and Dy7Rh3D28 at several temperatures.

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1-2-26

Quantum Phase Transition in the Solid Solution
Kitada A., Tsujimoto Y., Kageyama H., Yoshimura K., Nishi M.
Department of Chemistry, Graduate School of Science, Kyoto University; Institute for Solid
Staet Physics, University of Tokyo
The structure of (CuCl)LaNb2O7, ametastable phase prepared using an ionexchange reaction, consists of Cu2+Cl
layers sandwiched by non-magnetic
double-layered perovskite LaNb5+2O7
blocks. Thus it is regarded as an S =1/2 quasi-2D system. Previous magnetic
studies of this compound revealed thespin-singlet ground state with a zero-ﬁeld
gap of 2.3 meV to the low-lying triplet
excited states. The Br-based counterpart(CuBr)LaNb2O7 exhibits collinear antiferromagnetic (CAF) order at TN = 32 K
characterized by the propagation vector q= (pi, 0, pi). Apparently, the superexchangeinteractions through Cu-X-Cl (X = Cl,Br) substantially inﬂuence their magnetic
properties. The solid solution (CuCl1yBry)LaNb2O7 has been recently prepared
to investigate the correlation between thetwo states.15, 16 However, it should be
noted that (CuCl1-yBry)LaNb2O7 is subject to random disorder due to the differing
ionic radii of Cl and Br anions and that the
CuCl layer inherent to the magnetism isdirectly disrupted.
Thus we have decided to study the magnetism of (CuCl)LaTa2O7 and the solid
solution (CuCl)La(Nb1-xTax)2O7 [1. 2]. A
crucial advantage of studying the Nb-Ta
system (over the Cl-Br system) is that the
CuCl layers are unaffected by the substitution and that Nb and Ta ions have nearly
the same ionic radius (0.64 angstrom). We
observed persistence of the spin-singlet
state in (CuCl)LaNb2O7 up to x ˜ 0.4, accompanied by a slight reduction of the spin
gap with increasing x. (CuCl)LaTa2O7 exhibits collinear antiferromagnetic (CAF) order with TN ˜ 7 K, similar to what is observed in (CuBr)LaNb2O7. In the intermediate region (0.4 < x < 1), we observed

CAF order with a signiﬁcantly reduced
magnetic moment but with a nearly constant TN, suggesting that the CAF state coexists with the spin-singlet state in agreement with recent MuSR results.
References[1] A. Kitada et al., submitted to Phys. Rev.
B.
[2] Y. J. Uemura et al., submitted to Phys.
Rev. B.

Fig. 1.
Neutron diffraction of (CuCl)La(Nb1xTax)2O7 demonstrating the collinear (pi, 0, pi)magnetic order at low temperatures.

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1-2-27

Electric polarization ﬂop induced by magnetic phase transition in multiferroic
YbMn2 O5
H. Kimura1 , Y. Sakamoto1 , M. Fukunaga1 , Y. Noda1 , and H. Hiraka2
1 IMRAM, Tohoku University
2 IMR, Tohoku University
A rare-earth (R) manganite of RMn2 O5
is one of the typical multiferroic materials, which has been extensively studied[1].
However the origin of ferroelectricity is not
yet fully understood. We have recently
found in TmMn2 O5 the ﬂop of electric
polarization from b-axis to a-axis around5 K with decreasing temperature[2], whichis the ﬁrst discovery of a-polar phase in
RMn2 O5 system. It was reported previously that the polarization along b-axis disappear below ∼ 6 K in YbMn2 O5 [3]. Thisis a suggestive result being expected thepolarization ﬂop from b- to a-axis below∼ 6 K. We thus carried out neutron diffraction measurements and magnetic structure
analysis to clarify the microscopic magnetism in YbMn2 O5 .
Microscopic magnetic properties were
measured using AKANE spectrometer.
The results show that all the magnetic
phases which successively occur with decreasing temperature are incommensurate
and there is no commensurate magnetic
order at all in YbMn2 O5 unlike the other
RMn2 O5 families. Fig. 1(a) shows themagnetic Bragg peak proﬁles around Q =(2.55 4 0.265) taken at 2.5 K and 7 K,
showing the change of Bragg peak intensity. This indicates that the magnetic phasetransition takes place between 2.5 K and
7 K. We measured the electric polarizationof this material and found that, as shownin Fig. 1(b), the polarization ﬂop fromb- to a-axis occurs below ∼ 6 K, indicating the strong relevance between the direction of electric polarization and the magnetic structure. To clarify the microscopic
origin of this polarization ﬂop, we have
performed magnetic structure analysis inboth b-polar phase and a-polar phase using

FONDER diffractometer. A sufﬁcient number of the integrated intensities of magnetic
Bragg peaks were successfully measured atboth the phases. The magnetic structure
analysis is now in progress.
References[1] N. Hur et al.: Nature 429 (2004) 392.
[2] M. Fukunaga et al.: JPSJ 77 (2008) 094711.
[3] Y. Koyata et al.: JPSJ 65 (1996) 1383.

Fig. 1. (a) Peak proﬁles of magnetic Bragg reﬂection
around (2.55 4 0.265) of YbMn2 O5 taken at 2.5 K and
7 K. (b) Spontaneous electric polarization measured
along a- and b-axes as a function of temperature.

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1-2-28Relationship between Spin Helicity and Electric Polarization in Multiferroic
Material CuCrO2
Minoru Soda1, Kenta Kimura2, Tsuyoshi Kimura2, Masato Matsuura1 and Kazuma
Hirota1
1Department of Earth and Space Science, Graduate School of Science, Osaka University
2Division of Material Physics, Graduate School of Engineering Science, Osaka University
Ferroelectricity induced by a noncollinear
spin arrangement has been investigated experimentally and theoretically with respect
to delafossite CuCrO2. CuCrO2 undergoes
an antiferromagnetic transition at TN ˜25
K. A powder neutron diffraction study reported by H. Kadowaki et al. has indicatedthat CuCrO2 has an out-of-plane 120 deg.
magnetic structure below TN. [1] Within
the framework of the spin-current model,
an electric polarization P does not appear
macroscopically for this out-of-plane 120
deg. magnetic structure. However, the ferroelectricity has been recently reported in
the out-of-plane 120 deg. magnetic structure. [2,3] In the present work, the spinpolarized-neutron studies have been carried out on the multiferroic material CuCrO2 to clarify the relationship between
the spin helicity and the electric polarization P.
Below TN, the magnetic reﬂections wereobserved at Q-points (h /3,h /3,l) (hand h= 3n+1 or 3n+2 where n is integer). To discuss the magnetic domains, thecrystal was oriented with the [001] axis vertical, and the electric ﬁeld E was applied
to the [110] direction. (The intensities ofthe magnetic reﬂections with the neutron
spin parallel and antiparallel to the scattering vector are deﬁned as Ion and Ioff.)
After applying E=-73 kV/m, the difference
between Ion and Ioff was observed at all
the Q-points (1/3,1/3,0), (-1/3,2/3,0) and (2/3,1/3,0), although the relations between
Ion and Ioff at (-1/3,2/3,0) and (-2/3,1/3,0)
are opposite to that at (1/3,1/3,0). (The Qpoints (-1/3,2/3,0) and (-2/3,1/3,0) correspond to those rotated by 60 and 120 degrees from (1/3,1/3,0).)In the present CuCrO2 studies, the spin

helicities can be controlled by E without
the change of T. For E=-73 kV/m, Ioff
was larger than Ion at (1/3,1/3,0). The relation between Ion and Ioff was reversed
at (2/3,2/3,0). These results are consistent
with the helical magnetic structure or theout-of-plane 120 deg. magnetic structure.
At (-1/3,2/3,0) and (-2/3,1/3,0), Ioff was
smaller than Ion, which is opposite to thatat (1/3,1/3,0). For -73 kV/m < E < +73
kV/m, the sum of the spin helicities werereversible by the reversal of the electricﬁeld without changing T at all the Q-points(1/3,1/3,0), (-1/3,2/3,0) and (-2/3,1/3,0).
These results can be explained qualitatively
by a theoretical prediction proposed by T.
Arima.[4] However, for E > +73 kV/m,
the relation between Ion and Ioff at the Qpoint (1/3,1/3,0) changes. A large difference between Ion and Ioff was observed
not at (1/3,1/3,0) but at (-1/3,2/3,0). These
results indicate a possibility that the magnetic domains and the magnetic structures
are controllable by the electric ﬁeld.
[1] H. Kadowaki, H. Kikuchi and Y. Ajiro,
J.Phys.: Condens.Matter 2 4485 (1990)[2] S. Seki, Y. Onose and Y. Tokura, Phys.
Rev. Lett. 101 067204 (2008)[3] K. Kimura, H. Nakamura, K. Ohgushi
and T. Kimura, Phys. Rev. B 78 140401(R)(2008)[4] T. Arima, J. Phys. Soc. Jpn. 76 073702(2007)

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1-2-29Competition between Relaxor-like behavior and Magnetic Ordering in(1-x)BiFeO3-xBaTiO3Minoru Soda and Kazuma Hirota
Department of Earth and Space Science, Graduate School of Science, Osaka University
In relaxors, the temperature dependencesof the dielectric permittivity show a broad
maximum and a frequency-dependence.
Because the relaxors have the high dielectric constant around room temperature,they are industrially important. To explain
the T-dependences of the refraction indicesand the dielectric permittivity of the relaxor systems, Burns and Dacol proposed
the idea that randomly oriented, very local
polar regions start to appear below a characteristic temperature Td (Burns temperature). This Polar Nano Region (PNR) is
most important concept to consider the origin of the relaxor properties.
As a new example of such relaxor systems,
we have studied (1-x)BiFeO3-xBaTiO3.
Because (1-x)BiFeO3-xBaTiO3 with therelaxor-like dielectric property has themagnetic ions Fe3+, a question immediately arises as regards what magnetic
behaviors appear in this relaxor system. [1] In the present studies, the neutron scattering studies have been carried out on single crystalline samples
of 0.67BiFeO3-0.33BaTiO3(0.67BFO-BTO),
which is around Morphotropic Phase
Boundary(MPB), to clarify the relationship between relaxor-like dielectric property and magnetization.
Anisotropic nuclear diffuse scatterings,
which have disappeared at about 900 K,
have been observed around nuclear Bragg
reﬂections at T=550 K˜900 K. (The Tdependence of the dielectric permittivity of
0.67BFO-BTO shows a broad maximum at
Tmax=500 K˜700 K.) Although these nuclear diffuse scatterings are expected to indicate the existence of PNR, the change ofthese nuclear diffuse scatterings has been
observed below the antiferromagnetic transition temperature TN. The intensities ofthe magnetic Bragg reﬂections, which orig-

inate from G-type antiferromagnetic order,
begin to grow gradually at around TN˜500
K with decreasing T. Furthermore, the intensities of the nuclear Bragg reﬂections increase gradually below TN with decreasing
T. This increase of the intensities of the nuclear Bragg reﬂections corresponds to thedecrease of the nuclear diffuse scatterings
around them, indicating that the volume of
PNR decreases below TN. The simple Gtype antiferromagnetic order is expected tocompete with PNR and their domain walls.
We think that the crystal structure begins
to be formed regularly below TN with decreasing T. These results indicate the possibilities that the relaxor dielectric property and the antiferromagnetic order canbe controlled by the magnetic ﬁeld and theelectric ﬁeld, respectively.
Neutron scattering studies have been also
carried out on single crystalline sample
of 0.75BiFeO3-0.25BaTiO3(0.75BFO-BTO)
with no relaxor behavior. The magnetic
behavior of 0.75BFO-BTO is different fromthat of 0.67BFO-BTO. The magnetism of
0.67BFO-BTO is suppressed more than thatof 0.75BFO-BTO. For 0.75BFO-BTO withno relaxor behavior, PNR which are related
to the relaxor behavior are expected to besmall or few. The magnetic behavior of
0.75BFO-BTO is consistent with the ideathat the antiferromagnetic order competes
with PNR and their domain walls.
[1] M. Mahesh Kumar, A. Srinivas and S.
V. Suryanarayana, J. Appl. Phys. 87 (2000)
855.

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JAEA-Review 2013-039

1-2-30Magnetic structure analysis of Crednerite CuMnO2
Noriki Terada
National Institute for Materials Science
We also observed the magnetic diffuse
scattering above TN , suggesting the two dimensional character of CuMnO2 . For further investigation of the diffuse scattering,the inelastic neutron scattering measurements are desired.
References[1] M. Trari et al.: J. Solid State Chem. 178(2005) 2751.
[2] Y. Bessekhouad et al.:J. Mater. Sci. 42 (2001)
6469.
[3] J. Rodriguez-Carvajal: Physica B 192 (1993)
55.
3

40x10

CuMnO2 60 K
Antiferromagnetic phase: Q=(0.5,0.5,0.5)30

20Intensity

Crednerite CuMnO2 has a distinct two
dimensional crystal structure instructed byisosceles triangular lattice layers of themagnetic Mn3+ . Despite the large negative value of Weiss temperature θ p =−450 K, CuMnO2 exhibits the antiferromagnetic phase transition at relatively low
temperature TN = 64 K, which is reportedby the previous bulk measurements.[1, 2]
The further cooling produces the weekferromagnetic phase transition at 42 K.[1, 2]
Considering the two dimensional isosceles
triangular lattice crystal structure and therelatively large ratio between θ p and TN ,CuMnO2 is considered to be characterized
by the geometric frustration. Thus, a complex magnetic structure could be expectedin the low temperature phase. However,
the magnetic structural determination has
not been performed so far.
This time, in order to investigate magnetic orderings of CuMnO2 , we have performed the neutron powder diffraction
measurements. The experiments were carried out with the diffractometer HERMES
installed in the guide hall at JRR-3. The incident neutron wave length was 1.8204 Å.
The powder sample was mounted on thecold head of the closed cycle He refrigerator.
We have performed the rietveld reﬁnements for the data measured at the several
temperature from 10 K to 300 K, using FullProf reﬁnement program.[3] We observed
the magnetic Bragg reﬂection below 70 K
at the reciprocal lattice positions indexedas (h, k, l)±(0.5,0.5,0.5). The typical resultof the reﬁnements for the data measured
at 60 K, where the system is in the antiferromagnetic phase, is shown in Fig. 1.
The reﬁned magnetic structure is collinear
magnetic structure with the magnetic moments aligned to the direction perpendicular to the b axis (monoclinic unique axis).

10

0

-10
20

40

60

80

2-Theta (in degrees)

100

120

140

Fig. 1. Rietveld reﬁnement of the neutron diffraction
data obtained at 60 K for CuMnO2 .

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-31Long-time variation of magnetic structure in a multistep metamagnet CeIr3Si2
K. Motoya, Y. Muro and T. Takabatake (a)Tokyo University of Science, (a) Hiroshima University
with time. Neither the position nor the line
width of Bragg peaks showed appreciable
time variation. These results strongly suggest that we have observed the change ofthe volume fractions of two magnetic regions with a commensurate and an incommensurate structures.
We believe this is the ﬁrst real-time observation of magnetic structural change ina uniform magnetic system. In future experiments with high intensity apparatus,
we will be able to observe the change ofdomain size at very early stage of the time
evolution.
References[1] Y. Muro et al.: J. Mag. Mag. Mater. 310(2007) 389.
[2] K. Shigetoh et al. : Phys. Rev. B 76 (2007)
184429.

Amplitude (arb. scale)

400

MT-phase signal

300
4T=1 K, t*=3.8 x 10 s200

4

T=1.4 K, t*=1.7 x 10 s
100

0

3

T=1.9 K, t*=7.1 x 10 s
1200 0400LT-phase signal

1000
Amplitude (arb. scale)Time variation of magnetic property has
been extensively investigated in the spinglass study. In a system without randomness or imperfections we have not thought
to observe a time variation of magnetic
structures in an attainable time scale. We
report the ﬁrst observation of a long-timetransformation of magnetic structures in a
non-diluted magnet CeIr3 Si2 .
A ternary compound CeIr3 Si2 shows successive magnetic transitions at TN1 =4.1 K
and TN2 =3.3 K. At T < TN2 it shows
three-step metamagnetic transitions below
H=1.43 T.[1,2] When a sample is rapidly
cooled below TN2 , the magnetic Bragg
peaks corresponding to the medium temperature (MT) phase ( TN2 < T < TN1 )are observed. The amplitude of these Bragg
peaks gradually decreases as time goes on.
On the other hand, another group of Bragg
peaks corresponding to the low temperature (LT) phase ( T < TN2 ) gradually growwith time. Figure 1 shows the time variations of the amplitudes of the MT and LT
phase signals measured at various temperatures. At T=0.7 K the MT-phase signal wasobserved without detectable change up to
10 h and no LT phase signal was observed.
The time variations of the signal amplitude are well expressed by simple exponential functions with a characteristic timet∗ . The value of t∗ for each measurement is posted in the ﬁgure. We analyzed
the temperature variation of t∗ in terms of
the Arrhenius model. The activation energy of the time variation was obtained as
Ea /kB =4 K.
Although the magnetic structure in eachphase has not been determined, we presume that the transition from the MT phaseto the LT phase is basically an incommensurate to commensurate phase transition.
We note that in the present measurements,
only the amplitude of Bragg peaks varied

800
1200
Time (min)4
T=1.4 K, t*=1.2 x 10 s

1600

3

T=1.9 K, t*=5.5 x 10 s

800
600

4

400

T=1 K, t*=4.7 x 10 s

200
0
0

400

800
Time (min)

1200

1600

Fig. 1. Time variations of the amplitude of the MT
and LT phase signals at various temperatures.

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JAEA-Review 2013-039

1-2-32

Inelastic neutron scattering study in O2 adsorbed deuterated CPL-1
Takatsugu Masuda, Suguru Hondo an Masato Matsuuda
Yokohama City University, Osaka University
We have studied the spin dynamics ofoxygen molecules adsorbed in coordination polymers complex for a few years.
In the nano-scale porous O2 molecues
are aligned periodically and consequently
an articﬁcially designed O2 crystal isrealized. In case of {[Cu2(pyrazine-2,3dicarboxylate)2(pyz) ]2H2O}n abbreviatedas CPL-1 the O2 forms ladder-like structure. Previously we studied the magnetic
excitation of the adsorbed O2 molecule in
the protonated CPL-1 by inelastic neutron
scattering. Though we succeeded in extracting the main excitation of O2 (singlettriplet excitation at hw = J) by elaborate
data analysis, the huge background fromprotons smeared detailed information. Particularly we could not conclude the existence of the triplet-quintet excitation (presumed to be observed at hw = 2J) becauseof the poor signal noise ratio (signal/noise
˜ 1/10). In addition the obtained temperature dependence of the singlet-triplet excitation was of poor quality. Hence we
prepared 2 g of deterated CPL-1 sample
and performed inelastic neutron scattering.
We used PONTA spectrometer with horizontally focuse analyzer. The collimation
was open-80’-radial collimation-open and
Ef=14.7 meV. ORANGE type cryostat withspecially designed sample probe for O2 induction experiment was used.
The energy scans on non O2 adsorbed(ﬁlled circles) and O2 adsorbed (open circles) CPL-1 are shown in Fig. (a). A well deﬁned peak due to singlet-triplet excitation
is observed at 7.8meV. The energy is consistent with previous study on protonatedsample. The signal noise ratio is remarlably
improved. In Fig. (b) we show the net contribution of O2 molecule at T = 2 K and 60
K. No signal is observed at hw =2J ˜16meV.
This means that the O2 magnet realized in
the nanoporous is not a simple spin dimer

but probably a dimer magnet strongly coupled to lattice. Detail study on the exotic
magnet will be published elsewhere.
The difﬁculity of this experiment is that
we must collect a pair of scans on O2 adsorbed and O2 non-adsorbed samples forbackground subtraaction. Since the O2 adsorption process takes 12 hours, we perform all the presumably necessary scanson O2 adsorbed sample ﬁrst. Then we do
O2 de-adsorbtion process. After that wedo the scans on non O2 adsorbed sample.
The set of meaningful data can be obtained
after these steps, that is, the end of maschine time. After the experiment we foundthat temperature dependence data is notenough for publication. We will continue
this study in ﬁsical year of 2009.

Fig. 1. (a) Energy scans in O2 adsorbed and nonadsorbed CPL1. (b) Energy scans at T = 2 K and 60
K after background subtraction

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-33Chiral Helimagnetic Order in T1/3NbS2 (T=Cr, Mn)
Y. Kousaka1, Y. Nakao1, H. Furukawa2 and J. Akimitsu1
1Department of Physics and Mathematics, Aoyama-Gakuin Univ., 5-10-1 Fuchinobe,
Sagamihara 229-8558; 2Department of Physics, Ochanomizu Univ., 2-1-1 Ohtsuka,
Bunkyo-ku, Tokyo 112-8610
Systematic understanding of the interplay between a crystallographic structure
and magnetic order is an important issue
in the ﬁeld of magnetism. In particular,
the magnetic chirality triggered by crystallographic chirality has been discussed
as a long-standing problem. An intercalate system of 2H-NbS2 type chiral crystal structure T1/3NbS2 (T = transition
metal) has been paid attention as a candidate of chiral helimagnetic compounds. It
shows a variety of magnetic order; paramagnetic (T = Ti, V), ferromagnetic (T =Mn) and antiferromagnetic (T = Fe and Co).
Cr1/3NbS2 shows an magnetic anomaly ataround Tc ˜ 130 K and small-angle neutron
scattering experiments show helimagnetic
ordering.[1] While neutron diffraction in
Mn1/3NbS2 shows ferromagnetic, magnetization shows a magnetic anomaly as observed in Cr1/3NbS2.[2] Angle resolutionof thermal neutron diffraction experiments
is not high enough to separate fundamental
Bragg peaks and magnetic satellite peaks.
Therefore, Mn1/3NbS2 may be misinterpreted as a ferromagnetic ordering.
To examine the helimagnetic orderingin Cr1/3NbS2 and Mn1/3NbS2, we performed small angle neutron scattering experiments at SANS-U, a small-angle neutron scattering instrument with a 64 cmwide position sensitive area detector, installed at JRR-3M, Tokai, Japan. The wavelength of incident neutron beam was 11
A. The data was taken by using powder samples. The magnetic satellite peak
was detected by subtracting the room temperature data from the low temperature
data, though the intensity at lower q position is negative value due to failing tosubtracting paramagnetic scattering. Fig. 1
shows the observed magnetic peak posi-tion q and magnetic peak intensities. We
succeed in observing the magnetic satellite
peak, which indicates helimagnetic ordering with the pitch of 420 A for Cr1/3NbS2
and 700 A for Mn1/3NbS2. Therefore, themagnetic ordering in Mn1/3NbS2 is not
ferromagnetic, but helimagnetic.
[1] T. Miyadai et al.: J. Phys. Soc. Jpn. 52(1983) 1394.
[2] Y. Kousaka et al.: Nucl. Instr. and Meth.
A 600 (2008) 250.

Fig. 1. Magnetic peak position q and the peak intensity in (a) Cr1/3NbS2 and (b) Mn1/3NbS2

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-34

Neutron powder diﬀraction of Tb1-xGdxB2C2(x=0.15,0.2)
E. Matsuoka(A), Y. Sasaki(A), K. Ohoyama(B), H. Onodera(A)(A)Department of Physics, Tohoku University, (B)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 withrespect to the anomalous magnetic behavior, effects of substitution of Tb3+ ions by
Gd3+ have been examined and the T-x
phase diagram of Tb1-xGdxB2C2 has been
constructed [2]. The Gd substitution witha small content (x<0.075) induces drasticchange of magnetic properties, namely, anintermediate magnetic phase named AFM1
appears at TO<T<TN. Here, TO is a transition temperature from AFM1 to phase
IV. The neutron diffraction experiments of
Tb0.94Gd0.06B2C2 have revealed that themagnetic structure of AFM1 phase is along periodic one whose wave vector is[1+delta delta 0] with delta˜0.114 [3]. The
magnetic structure below TO (phase IV) is
described by the main wave vector of [1 0
1/2] in addition to the long-periodic component [3]. The results of neutron diffraction support the assumption proposed inref. [2] that the antiferro-octupolar (AFO)
order occurring at TO forces to align themagnetic moments with their wave vector of [1 0 1/2]. This assumption explains
satisfactorily the anomalous properties of
TbB2C2 and the Gd-substitution effects [2].
TO decreases very rapidly and disappears at x = 0.075, while TN increases
with x. For compounds with x > 0.075, a

new transition temperature T1 appears below TN. Although the magnetic phase forT1<T<TN is considered to be the sameto AFM1 phase described above, that forT<T1 is not phase IV. The magnetic phase
below T1 is called as AFM2 [2]. In thisstudy, neutron powder diffraction experiments of Tb0.85Gd0.15B2C2 (x = 0.15) havebeen performed using HERMES installedat the JRR-3M reactor in JAEA to determine
the magnetic structures for T1<T<TN and
T<T1. Neutrons with a wavelength of
1.8204(5) A were obtained by the 331 reﬂection of the Ge monochromator. Since thenatural boron is a strong neutron absorber,the 11B-enriched boron was used for the
sample preparation.
Fig. 1 shows the neutron diffraction
patterns of Tb0.85Gd0.15B2C2 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 (101)and (211) are observed at 17 K (T1<T<TN)as shown in Fig. 1(b). The positions of thesesatellite peaks can be explained by considering a long periodic one whose wave
vector is [1+delta delta 0] with delta˜0.11,
implying that the magnetic structure at
T1<T<TN is almost identical to AFM1 for
Tb0.94Gd0.06B2C2. These satellite peaks
disappears at 3.8 K and the other magnetic Bragg peaks appears as shown in Fig.
1(c). The magnetic Bragg peaks at 3.8 K(T<T1) can be explained by considering
the wave vector of (100). Therefore, themagnetic structure of AFM2 is identical tothat of GdB2C2.
[1] K. Kaneko et al., J. Phys. Soc. Jpn. 70(2001) 3112.
[2] E. Matsuoka et al., J. Phys. Soc. Jpn. 75

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JAEA-Review 2013-039(2006) 123707.
[3] Y. Sasaki et al., to be published in Physica B.
[4] Y. Yamaguchi et al., Appl. Phys. A 74
[Suppl.] (2002) S877.

Fig. 1. Neutron powder diffraction patterns of
Tb0.85Gd0.15B2C2 measured at several temperatures.

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1-2-35

Elastic diﬀuse scattering of neutrons in Fe3Pt Invar alloys
M. Takasaka, Y. Tsunoda
School of Science and Engineering, Waseda University, 3-4-1 Ohkubo, Shinjuku-ku, Tokyo
169-8555
Very recently, we have found elastic diffuse scattering of neutrons around various Bragg peak positions for the typical Invar alloys Fe1-XNiX (0.35<X<0.60) alloys.
The scattering intensities depend on temperature and Ni concentration and increase
with decreasing temperature and decrease
with increasing Ni concentration. Since theranges of temperature and Ni concentration, for which diffuse scattering is observed, coincide with those for which theInvar anomalies are observable, the diffuse scattering seems to have strong correlations with the Invar effect. The experimental data were well reproduced as diffuse scattering due to the formation of clusters with the local lattice deformation wave
propagating along the <1 1 0> direction
and the <1 -1 0> polarization vector. Since
an Fe65Ni35 Invar alloy is located close
to the phase boundary of fcc-bcc martensitic transformation, the origin of the diffuse scattering would be explained as a
pre-martensitic phenomenon of an fcc-bcc
phase transition of the alloy.
Another archetypical Invar alloys, ordered
and disordered Fe3Pt alloys are also located close to the phase boundary of anfcc-bcc martensitic transformation. Thus,
we can expect similar diffuse scattering forthese Invar alloys. We report observationof similar elastic diffuse scattering of neutrons for ordered and disordered Fe3Pt Invar alloys as those for the FeNi alloys. The
experimental data were analyzed using the
Huang diffuse scattering. In Fig 1, diffuse
scattering observed around (200) for ordered Fe72Pt28 alloy and calculated one
using the expression of Huang diffuse scattering are given. This pattern is very similar to that observed for the Fe65Ni35 alloy. Since the similar diffuse scattering isobserved for the disordered Fe72Pt28 al-

loy, appearance of elastic diffuse scattering is a common feature of typical Invar
alloys, ordered and disordered Fe3Pt andFe1-xNix (0.35<x<0.5). Various anomalous
magnetic behaviors have been reported byprevious authors as common properties for
the Invar alloys. The local lattice deformation observed here would give a strong
effect to the magnetism of the Invar alloys. Spin modulations coupled with thelocal lattice deformation would be the future problem.

Fig. 1. Fig.-1 Observed and calculated diffuse scattering around (2 0 0)

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-36

Reﬁnement of magnetic structure in the ferroelectric phase of Cu(Fe,Ga)O2
T. Nakajima1 , S. Mitsuda1 , K. Yoshitomi1 , H. Kimura2 , Y. Noda2
1 Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601
2 Institute of Multidisciplinary Research for Advanced Materials, Tohoku Univ., Sendai

980-8577
Delafossite compounds CuFeO2 (CFO),
CuFe1− x Alx O2 (CFAO) and CuFe1− x Gax O2
have been the subjects of increasing recent interest as a magneto-electric (ME)multiferroics, because of the discovery of
the ferroelectricity in the ﬁeld-induced or
impurity-induced phase from the groundstate.[1, 2] In the previous study, we havereported that the magnetic structure in
the ferroelectric phase of these systems is
a ’proper-screw-type’ magnetic structure
shown in Fig.1(a),[2] suggesting that theorigin of the ferroelectricity is not the ‘spincurrent’ model but the d-p hybridization
model.[3] However, the previous measurements was not so sensitive to the directionof the helical axis and the ellipticity of themagnetic structure. In order to conﬁrm theorigin of the ferroelectricity in this system,
it is critical to reﬁne the magnetic structuralparameters in detail. In the present measurements, therefore, we have performed
precise reﬁnement of the magnetic structure using 4-circle neutron diffraction anda single-crystal CFGO (x = 0.035) sample,
which exhibits the ferroelectric phase under zero magnetic ﬁeld.
The neutron diffraction measurements
were performed using the four-circle neutron diffractometer FONDER installed at
JRR-3 in JAEA. The incident neutron beamwith wavelength 1.239 Å was obtained by aGe(311) monochromator. The sample wasmounted on a closed-cycle He-gas refrigerator.
For the magnetic structure analysis, wehave measured integrated intensities ofmore than 130 magnetic Bragg reﬂections
at T = 2.8 K and 6.5 K. The effect ofneutron absorption was corrected by the
DABEX software. Using a homemade
least-square ﬁtting program, we have re-ﬁned the lengths of the magnetic moments
along x and z axes (μ x and μz ), the phaseshift in the magnetic modulation (δ), andthe direction of the helical axis. As a result, the direction of the helical axis was determined to be parallel to the b-axis within
the experimental accuracy, and the ellipticity and the phase shift were determined tobe μ x /μz = 0.895 and δ = 73.4◦ at T = 2K,
respectively. These results strongly conﬁrm that the origin of the ferroelectricity inthis system is not the ‘spin-current’ modelbut the d-p hybridization model.[3] We also
found that the ellipticity and the phase shiftslightly decrease with increasing temperature. More comprehensive analysis including results of spherical neutron polarimetry
will be published elsewhere.
References[1] T. Kimura et al.: PRB 73 220401(2006).
[2] T. Nakajima et al.: JPSJ 76 043709 (2007).
[3] T. Arima: JPSJ 76 073702 (2007).

Fig. 1. (a) Magnetic structure in the ferroelectric phase. [(b)-(c)] Comparison between | Fcal | and| Fobs | obtained from the magnetic structure analysis
at (b) T = 2.8 K and (c) T = 6.5 K.

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JAEA-Review 2013-039

1-2-37

Magnetic Structure in Ba2 Mg2 Fe12 O22
H. Sagayama(A), K. Taniguchi(A), T. Arima(A), Y. Nishikawa(B), S. Yano(B), J.
Akimitsu(B), H. Kimura (A), Y. Noda(A)(A)IMRAM, Tohoku Univ., (B)Dept. Phys., Aoyama-Gakuin University
It has been recently found that a Ytype hexaferrite Ba2 Mg2 Fe12 O22 (BMFO)
exhibits a nonlinear magnetoelectric effect[1,2]. It is proposed that the conical magnetic structure at low temperatures is modiﬁed by the application of a weak magnetic
ﬁeld perpendicular to the cone axis of thec axis, which produces the electric polarization. To reveal the correlation between
the magnetic structure and the electric polarization in the presence of magnetic ﬁeld,
we carried out a magnetic structure analysis of a single crystal of BMFO with H  b∗ .
Single crystals of BFMO were grownfrom Na2 O-Fe2 O3 ﬂux. Neutron diffraction
measurement was performed with a fourcircle neutron diffractometer FONDER at
JRR-3. A single crystal was set in a magnetic ﬁeld of about 0.3 T between two permanent magnets. The direction of the magnetic ﬁeld was parallel to the b*-axis. The
crystal was then cooled down to 4 K. Proﬁles of 397 fundamental reﬂections and 105
pure magnetic reﬂections with the magnetic modulation vector Q=(0 0 3/2) were
measured.
From the least-square ﬁt of the intensities of the pure magnetic reﬂections, we determine the antiferromagnetic component
with a period of 2/3 c. Figure 1 shows the
projection of the magnetic structure along
the magnetic ﬁeld. It clearly shows thenoncollinear nature of the magnetic structure. In fact, the spin current model [3] orthe inverse Dzialoshinskii-Moriya interaction [4], deﬁned as

References[1] K. Taniguchi et al., Appl. Phys. Express 1, 031301 (2008).
[2] S. Ishiwata et al., Science 319, 1643
(2008).
[3] H. Katsura et al., Phys. Rev. Lett. 95,
057205 (2005).
[4] I. A. Sergienko and E. Dagotto, Phys.
Rev. B 73, 094434 (2006).

Δpij ∝ eij × (Si × S j ),can explain the macroscopic electric polarization along the a-axis. Here, Δpij is a local electric polarization induced by a nonlinear pair of adjacent spin moments Si and
S j , connected by a unit vector eij .
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JAEA-Review 2013-039

1-2-38Eﬀective random-ﬁed domain-state in Ga-substituted CuFeO2
T. Nakajima, S. Mitsuda, M. Yamano, H. Yamazaki, K. Kuribara
Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601
The effects of random ﬁeld on the stability of a long-range magnetic ordering havebeen extensively studied from 1980s. In
the early stage, the random-ﬁeld effect was
experimentally investigated using diluted
antiferromagnets under applied magnetic
ﬁeld.[1] The recent experimental studies on
CsCo1− x Mgx Br3 have revealed that a combination of a partially-disordered magnetic
structure, which often shows up in somemagnetically frustrated systems, and siterandom magnetic vacancies can generate’effective-random-ﬁeld’ without an application of external magnetic ﬁeld.[2]In the previous works, we have foundthat CuFe1− x Alx O2 (x > 0.10) exhibits
the effective random-ﬁeld domain-state, inwhich the local magnetic structure is a sinusoidally amplitude modulated incommensurate structure.[3] We also found thatthe scattering function S(q) broadens as
the Al-concentration increases. This indicates that the magnetic correlation lengthis shortened by the Al-substitution. However, the recent studies on CuFe1− x Gax O2
have pointed out that the Al-substitution
produces not only the magnetic vacancies
but also local lattice distortions due tothe difference between the ionic radii of
Fe3+ and Al3+ .[4] Although this local distortion might disturb the long-range magnetic ordering, this should be distinguishedfrom the effective random-ﬁeld effect. In
order to purely investigate the effective
random-ﬁeld effect, in the present study,
we used Ga-substituted CuFeO2 samples,in which the local lattice distortion is relatively small.
We performed neutron diffraction measurements on CuFe1− x Gax O2 samples withx = 0.20 and 0.30, 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 in-cident neutron is 2.44 Å. The single crystalof CuFe1− x Gax O2 samples were mounted
in a 4 He-pumped cryostat with a hexagonal ( H, H, L)-scattering plane. In orderto evaluate the magnetic correlation length
quantitatively, we analyzed the scattering
proﬁle, using Multi-Proﬁle-Deconvolution(MPD) method presented in Ref. [3].
Figures 1(a) and 1(b) show the( H, H, 3/2) diffraction proﬁles at T = 2.0K
and results of the MPD-analysis. For both
samples, the functional form of S(q) are
well described by the sum of a Lorentzianterm and Lorentzian-Squared term shownin Fig. 1(c). The Lorentzian-squared
component dominating at low temperature indicates the domain state as seenin the prototypical random-ﬁeld Isingmodel.[1] While the ratio between theamplitudes of Lorentzian and Lorentziansquared terms are comparable to eachother (B/A = 0.02 ∼ 0.09), the widthsof S(q) are rather different. The further
detailed analysis is now in progress.
References[1] D. Belanger et al.: PRB 31 4538 (1985).
[2] J. van Duijn et al.: PRL 92 077202 (2004).
[3] T. Nakajima et al.:JPCM 19 145216 (2007).
[4] N. Terada et al.: PRB 78 014101 (2008) .

Fig. 1. [(a)-(b)] ( H, H, 3/2) diffraction proﬁles of(a) x = 0.20 sample and (b) x = 0.30 sample at
T = 2.0K, and results of the MPD-analysis.(c) The
deﬁnition of the functional form of the scatteringfunction S(q).

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JAEA-Review 2013-039

1-2-39Competing Interactions in Two Dimensional Square Lattice CuSb2-xTaxO6
M. Nishi, M. Kato(A) and K. Hirota(A)ISSP Univ. of Tokyo, (A)Inorganic Chemistry Lab. Doshisya Univ.
CuSb2O6 compound has a tri-rutile typestructure in which Cu2+ ions form a squarelattice [1]. The magnetic susceptibility of
CuSb2O6 indicates a typical behavior for
S=1/2 one-dimensional Heisenberg antiferromagnet above 20K and shows a antiferromagnetic (AF) long-range order at 8.7
K in which Cu spins are 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 than next nearest coupling J2along diagonal, Neel order will be stabilized. Then J2 interaction through Cu-O-OCu bond is dominant on the collinear orderof CuSb2O6. The substitution of Ta atom instead of Sb atom causes the decreasing oftransition temperature of long-range orderwhich disappears above x=1 [4]. TaO6 octahedron occupies inter CuO layers and theinter layer coupling may be decreased withthe 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 AF, there are the spin
frustrations between J1 and J2 couplings
even if J1 coupling is ferromagnetic or AF[5].
The results of ﬁrst neutron inelastic scattering measurements of CuSbTaO6 powder samples were reported at last year(#461, #464) that the magnetic spin gap
was observed at 0.8 meV with the use of
PONTA (5G) spectrometer. High energy
resolution experiments were done for the
conﬁrmation of the spin gap by the cold
neutron triple-axis spectrometer HER (C11)
installed at the JRR-3M reactor at JAEA.
Magnetic excitation peak was observed at
Q=0.6A-1 for constant E=0.4 meV, 1.0 meV
and 1.4 meV scans at the temperature 5K
as shown in ﬁgure 1. The spin gap in magnetic scattering could not be observed withthe energy resolution 0.14 meV. This re-sult indicates that CuSbTaO6 is typical onedimensional magnetic substance. The peak
position along Q is near 0.6 A-1 in deviation from the expected value 0.4735 A-1 in
Cu-O-O-Cu chain.
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 by the cold neutron-scattering. Magnetic
spin gap was not observed and the peak by antiferromagnetic correlation was observed at several constant E-scan.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 873- 115 -

JAEA-Review 2013-039

1-2-40Spin-driven dielectric relaxation in a paraelectric phase of magneto-electric
multiferroic CuFeO2
S. Mitsuda , M. Yamano , K. Kuribara , T. Nakajima , K. Masuda, and K. Yoshitomi
Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601
Magnetic oxide CuFeO2 is a raremagneto-electric
multiferroic
wheremagnetic ﬁeld-induced or nonmagnetic
impurity-induced proper helical magnetic
ordering generates a spontaneous electric polarization. We have measured thecomplex permittivity in various magnetic
phases under an applied magnetic ﬁeld
up to 15 T, and found Debye-type-likedielectric dispersion with low relaxation
frequency in only 4-sublattice(4SL) antiferromagnetic ground state. The relaxation
frequency of dielectric dispersion showsinteresting anisotropic magnetic ﬁeld aswell as temperature dependences. Although so-called Maxwell-Wagner effectin a dielectric system with heterogeneous
nature can often explain this kind of magnetodielectric effect [1], we speculated that
4SL-speciﬁc magnetic domain wall motion
must be responsible for the dielectricdispersion; As shown in Fig. 1(a), themagnetic domain wall moving back andforth, and corresponding displacement ofoxygen near magnetic domain wall can be
responsible for the dielectric dissipation.
Here, we consider the magnetic domain
wall is essentially the same as AD-type
domain wall discussed in domain growth
kinetics in the isosceles triangular Ising
antiferromagnet CoNb2 O6 [2].
In order to check the existence ofthe magnetic domain state in 4SL phaseof CuFeO2 , we have performed neutron diffraction experiments to determine the functional form of the scattering function, using the triple-axis neutron spectrometers HQR(T1-1) installedat JRR-3. The collimation open-’40-’40’40 was employed, and the wavelengthof the incident neutron was 2.44 Å. As
shown in Fig. 1(b), scattering proﬁle of
4SL (1/4, 1/4, 3/2) magnetic reﬂection isentirely different from resolution-limited
Gaussian and rather close to Lorentziansquared speciﬁc to the magnetic domainstate. The further detailed analysis using
Multi-Proﬁle-Deconvolution method [3] is
now in progress.
References[1] G. Catalan, APL. 88, 102902 (2006).
[2] S. Kobayashi et al., PRB 69, 144430 (2004).
[3] T. Nakajima et al.:JPCM 19 145216 (2007).

Fig. 1. a) Schematic drawings of magnetic domain
wall moving back and forth, (b) scattering pro?le of
4SL (1/4, 1/4,3/2) magnetic reﬂection.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 886- 116 -

JAEA-Review 2013-039

1-2-41

Inelastic Neutron Scattering Study on Triangular Lattice Antiferromagnet CuCrO2
T. Nozaki, K. Hayashi, and T. Kajitani
Department of Applied Physics, Graduate School of Engineering, Tohoku University, Sendai,
980-8579
Delafossite-type oxide CuBO2 has received much attention as a model materialof the magnetically frustrated triangularlattice antiferromagnets. CuFeO2 reaches
Ising-like antiferromagnetic state thorough2-step phase transitions at TN1 = 14 K andTN2 = 10.5 K. On the other hand, CuCrO2
shows Heisenberg-type antiferromagnetic
state below TN = 24 K. Recently both systems have been intensively studied due tothe local ferroelectric polarization[1,2]. Previously we measured the inelastic neutron
scattering (INS) spectra of CuFeO2 powder.
Below 12.5 K the INS peaks corresponding
to the creation of localized magnon mode
were observed. Above 11 K, the quasielastic neutron scattering (QNS) peak was
observed. In this study, we measure the
INS spectra of CuCrO2 powder using acold neutron spectrometer, AGNES (C3-11), to compare the magnetic behavior with
CuFeO2 .
Figure 1 shows neutron scattering intensity, S( E), being the summation of
S(|Q|, E) in the Q-space of CuCrO2 powder taken at 10, 20, 30, and 150 K. In the
CuCrO2 case, only the QNS peak is observed. The maximum QNS intensity is observed at 30 K, just above TN . Below 30 K,
the QNS intensity exists in the Q-space below |Q| = 1.5 A−1 . In comparison, the QNS
intensity at 150 K appears in the observed
Q-space, conceivably due to the Heisenberg paramagnetic scattering. For further
understanding of the corresponding spin
dynamics, INS measurements on CuFeO2
and CuCrO2 using the triple-axis spectrometer HER (C1-1) is underway.
References[1] T. Kimura, J. C. Lashley, and A. P.
Ramirez: Phys. Rev. B 73 (2006) 220401.
[2] S. Seki, Y. Onose, and Y. Tokura: Phys.
Rev. Lett. 101 (2008) 067204.

Fig. 1.
Inelastic neutron scattering spectra of
CuCrO2 powder at 10, 20, 30, and 150 K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 897- 117 -

JAEA-Review 2013-039

1-2-42

Observation of magnetic ﬂuctuation in Ni2(OD)3Cl by neutron scattering
Y. Oohara1, M. Hagihala2, X.G. Zheng2
1, ISSP, Univ. of Tokyo, 2, Faculty of Sci. and Engineer. Saga Univ.
As the temperature is decreased, conventional magnetic materials exhibit a slowing down of the magnetic ﬂuctuations
as the temperature approaches the critical point, Tc (namely the critical slowing
down). Crossing Tc, the ﬂuctuations disappear rapidly and the magnetic moments
are frozen into static at T << Tc. All conventional magnetic materials of ferromagnets, antiferromagnets or spin glasses arefeatured by the freezing of magnetic moments into static. Recently there are reported new dynamical magnetic states ofspin ice and spin liquid in rare earth pyrochlores where magnetic ﬂuctuation persist down to 0 K. However, these states arebasically disordered and do not have an order over a macroscopic range (long rangeorder). It is believed that a long range order in magnet must be fully frozen (static).
However, recently we observed an exotic dynamical antiferromagnetic order below TN=4.5K in Ni2(OH)3Cl by muon spin
relaxation (1). The present neutron scattering study was designed to further investigate this magnetic order. Elastic and inelastic measurements were performed at
HQR and HER, respectively, at JAEA. The
elastic measurement showed a clear longrange order extending over a spacing ofapproximately 56 (Fig. 1). Inelastic measurements suggested spin ﬂuctuation of 0.5
meV at 0.8 K, which is less than 1/5 of its
transition temperature. The analysis to reveal its magnetic structure is in progress.

Fig. 1. Elastic scattering data showing magnetic reﬂections in the ordered state. The inset plot showsthe evolution of two magnetic peaks below TN.

References:[1] X. G. Zheng, M. Hagihala, K.
Nishiyama, T. Kawae,Physica B 404(2009) 677-679.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 901- 118 -

JAEA-Review 2013-039

1-2-43

Study of spin gap in two-dimensional frustrated triangular lattice: YbAl3C3
M. Kosaka(A), T. Kobiyama(A), A. Yamada(A), K. Ohoyama(B), N. Aso(C)(A)Grad. School of Sci. and Engi., Saitama Univ., (B)IMR Tohoku Univ., (C) ISSP-NSL Univ.
Tokyo

1000
YbAl3C3
HER
Ef = 2.4 meV
q = 1.3 Åí1
T = 0.7 K

800
Intensity (arb. Units)

YbAl3C3 shows the highly frustrated
phenomena with a spin gap. The inelastic neutron spectra of low-lying magnetic excitations at low temperatures arequite similar to those of SrCu2(BO3)2and (CuCl)LaNb2O7 that exhibit a dimer
ground state in a two-dimensional quantum spin system. In order to investigate low-lying magnetic excitations at low
temperature, we performed inelastic neutron scattering (INS) measurements on the
triple-axis spectrometer C1-1 (HER) installed at the JRR-3M reactor. The collimations after the monochromator were open(Sample)-radial collimator-open.
Figure 1 shows the spectra measured using Ef=2.4 meV with a high resolution of
0.06 meV at T=0.7 K. As a result, it became
clear that the ﬁrst excited state consists ofthree excitations and the second excitedstate is composed of many excitations. The
solid line shows the least-squares ﬁt to theexperimental data where the peaks are approximated by three Gaussian curves. The
excitation energies are estimated to be 1.22,
1.42, and 1.62 meV using the same full
widths at the half maximum of 0.18 meV.
In single crystalline SrCu2(BO3)2, the three
resolved branches of the triplet excitation,
which are attributed to the DzyaloshinskiMoriya interaction, were observed by highresolution INS experiments. The crystal
symmetry of YbAl3C3 lowers below thephase transition at 80 K; this will satisfy thecondition of the Dzyaloshinski-Moriya interaction. When we consider the analogy
between the results of the INS measurements for these two compounds, the ﬁrst
and the second excitations are expected tobe the single-triplet excitations and twotriplet excitations, respectively. Moreover,the energy gaps, Δ1  1.5 and Δ2  2.9
meV, satisfy the relation Δ2 ≈ 2Δ1 .

600
400
200
0
1.0

1.5

2.0
2.5
Energy Transfer (meV)

3.0

3.5

Fig. 1. Detailed inelastic neutron spectra of YbAl3C3
at 0.7 K with Ef=2.4 meV. The full curve represents
the least-squares ﬁt where the peaks are approximated by three Gaussian curves.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 910- 119 -

JAEA-Review 2013-039

1-2-44Spin Waves in MnPS. Yano(1) , M. Nishi(2), M. Matsuura(3), K. Hirota(3) 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(3)Department of Earth and Space Sceince, Graduate School of Science
Manganese phosphide MnP is a ferromagnetic intermetallic compound below TC =291K, and it transforms into a proper screw
state at T* = 47K.
The crystal structure is a slightly distorted
NiAs structure with the lattice parametersof a = 5.916 , b = 5.260 , c = 3.173
at room temperature. In the ferromagnetic
state, the easy-axis of the magnetization isthe c-axis. In the proper screw state, thespin rotates in the b-c plane with a propagation vector δ = 0.117a* along the a-axis.
One of our interests of MnP is the mechanism of transition from ferromagnetism
to helimagnetism which had not been explained by theoretical viewpoint. In order
to elucidate the mechanism, the information of spin wave in the whole Brillouinzone is crucially important.
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 temperaturedependence, and also the quadratic q dependence was observed both along the band c-axes. In the proper screw state, spinwaves along the a- and b-axes had beenmeasured by Tajima et al[2]. They reported
the anomalous jump around T* along thea-axis which may be related to 3 δ.
In order to obtain the spin wave dispersion relations, we performed the neutron
inelastic scattering experiments at tripleaxis spectrometer PONTA (5G), JRR-3M reactor in JAERI (Tokai).
The single crystal of MnP, whose size
is 9mm φ× 40mm, was grown by the
Bridgman method.
The spin wave dispersions have been mearsured along the a-axis at 12 K and 50K, as
shown in Fig1. We could observe the spinwave dispersions along the a-axis, however, anomalous jump around T* which
Tajima et al reported was not found. It is
probably broadened dispersion due to itinerant magnetism.
In order to obtain the spin waves in thewhole Brillouin zone, further measurements of spin waves at higher energy (˜100meV) and lower energy (0 ˜ 2 meV) are
now in progress.

References[1] Y Todate et al.: Jou Phys Soc Jpn. 56 36(1987).
[2] K Tajima et al.: Jou Mag Mag Mat. 15-18
373-374 (1980).

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

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 914- 120 -

JAEA-Review 2013-039

1-2-45Spin Waves in MnPS. Yano(1) K. Iwasa(2) and J. Akimitsu(1)(1)Department of Physics and Mathematics, Aoyama-Gakuin Univ., 5-10-1 Fuchinobe,
Sagamihara (2) Department of Physics, Tohoku University, Sendai 980-8587
Manganese phosphide MnP is a ferromagnetic intermetallic compound below TC =291K, and it transforms into a proper screw
state at T* = 47K.
The crystal structure is a slightly distorted
NiAs structure with the lattice parametersof a = 5.916 , b = 5.260 , c = 3.173
at room temperature. In the ferromagnetic
state, the easy-axis of the magnetization isthe c-axis. In the proper screw state, thespin rotates in the b-c plane with a propagation vector δ = 0.117a* along the a-axis.
One of our interests of MnP is the mechanism of transition from ferromagnetism
to helimagnetism which had not been explained by theoretical viewpoint. In order
to elucidate the mechanism, the information of spin wave in the whole Brillouinzone is crucially important.
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 temperaturedependence, and also the quadratic q dependence was observed both along the band c-axes. In the proper screw state, spinwaves along the a- and b-axes had beenmeasured by Tajima et al[2]. They reported
the anomalous jump around T* along thea-axis which may be related to 3 δ.
We performed the neutron inelastic scattering experiments at triple-axis spectrometer TOPAN (6G), JRR-3M reactor in JAERI(Tokai).
The single crystal of MnP, whose size is
9mm φ× 40mm, was grown by the Bridgman method.
The spin wave dispersions have been measured along the a-axis at 14 K, 35K, 54K
and 81K, as shown in Fig1. The dispersion
curve below T*, there seems to be two lines.
However, the indicated lines by an arrow

are arised from another Brillouin zone.
In order to obtain the spin waves in thewhole Brillouin zone, further measurements of spin waves at higher energy (˜100meV) and lower energy (0 ˜ 2 meV) are
now in progress.

References[1] Y Todate et al.: Jou Phys Soc Jpn. 56 36(1987).
[2] K Tajima et al.: Jou Mag Mag Mat. 15-18
373-374 (1980).

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

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 915- 121 -

JAEA-Review 2013-039

1-2-46

Research for magnetic reﬂections on HoRh2Si2
T. Shigeoka(A), A. Tanaka(B), G. Nakamoto(C)(A) Grad. Sch. of Sci. Eng. Yamaguchi Univ, (B) Grad. Sch. of Sci. Eng. Hiroshima Univ.
(C)Japan Advanced Institute of
The ternary compound HoRh2Si2 crystallizes in the tetragonal ThCr2Si2-type
crystal structure (space group: I4/mmm).
It shows an antiferromagnetic order below TN=29.5 K. Recent magnetic study
shows that HoRh2Si2 has three transitions:
T1=12.4 K, T2=27.5 K and TN=29.5 K. The
neutron diffraction study were performed
on a single crystal compound and following results have been reported [1]; at
low temperatures below T1, an appearanceof antiferromagnetic reﬂections associatedwith the propagation vector k= (0, 0, 1) has
been conﬁrmed. Both (001) and (100) reﬂections are observed, indicating that magnetic moments tilt from the c- and a-axis.
This result is consistent with the previous
report [2]. The (001) reﬂection disappears
above T1. The temperature dependency ofintensity 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 T2<T<TN. Thus neutron study
has been carried out on a powdered sample for 4K-35K by using the HERMES spectrometer of JRR-3M with wave length of
1.82645 A.
For low temperatures, the previous results have been conﬁrmed; the antiferromagnetic structure with the propagation
vector k= (0, 0, 1) appears below T2.
Neutron diffraction patterns above T2 areshown in Fig. 1. New antiferromagnetic reﬂections (indicated by arrows) appear, indicating a change of the magnetic structure at T2. The detail analysis is now inprogress.

References[1] T. Shigeoka et al., Activity report on
Neutron Scat. Res. Vol.14 (2008)[2] M. Slaski et al., J. Magn. Magn. Mat.
39(1983)268.

Fig. 1. Neutron diffraction patern at 28 K below TN.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 922- 122 -

JAEA-Review 2013-039

1-2-47

Neutron scattering study on the magnetic moleculars
K. Iida A , H. IshikawaB , T. YamamseB , T. J SatoB
A ISSP, B Dept. of Phys. Tokyo Inst. of Techcalculated scattering intensitys are shownin Figs. 1 (a) and 1 (b) using the solid lines:
a good coincidence with the observation
can be readily seen. This satisfactory correspondence ensures the reliability of the estimated parameters.
By ascribing the 0.8 meV peak to a superposition of four magnetic excitations between two Stotal = 1/2 and two Stotal =3/2 doublets, we have successfully estimated the anisotropic as well as the antisymmetric interactions. And this result isthe evidence that the DM interaction exsist
in V3 .
[1] K. Y. Choi et al., Phys. Rev. Lett. 96,
107202 (2006)[2] T. Yamase et al., Inorg. Chem. 43, 8150
(2004).
(a) (b)500

500

Intensity (counts/85min.)

400

3  

y y 
H = − ∑ J x six six+1 + si si+1 + J z siz siz+1

400

300

200

300

-1

-1

Ef=2.4 (meV), Q=0.85 (Å )0.7 (K),
5.4 (K)
resolution function
subtraction
calculation

Ef=3.0 (meV), Q=0.6 (Å )0.9 (K),
30 (K)
resolution function
subtraction
calculation

200

100

100

0

0

0.5

0.6

0.7

0.8

0.9

1.0 0.5

0.6

0.7

0.8

0.9

Intensity (counts/20min.)Several triangular spin clusters showed
an attractive phenomenon, that is a halfstep magnetization change with hystersis.
The avoided level crossing between the
Stotal = 1/2 and Stotal = 3/2 states dueto the DM interaction is suggested to be
the origin of the half-step change [1]. Oneof such molecular nanomagnets exhibiting
the half-step change is the V3 molecular
nanomagnet [2]. Although the DM interaction is of particular importance in these system, there are no report on the DM interaction using the microscopic method. Hence,
we have performed an inelastic neutron
scattering (INS) to investigate the DM interaction.
Approximately 0.7 grams of deuterated
powder sample were used in our INS experiments on HER. We plotted INS spectra in the range of 0.5 ≤ h̄ω ≤ 1.0 meV in
Fig. 1 (a). At lower temperature, the intensity around h̄ω = 0.8 meV apparently grew
up. In contrast, the peak almost disappears
at 5.4 K, and there remains only the incoherent component in the INS spectrum.
Same results were obtained on E f = 3.0
meV as shown in Fig. 1 (b). As a model
Hamiltonian, we here propose the following form consisting of anisotropic exchange
and DM interactions and the Zeeman term;

1.0

Energy transfer (meV)

i =1

3
 x y
y x 
z
+ ∑ Di,i+1 s i s i +1 − s i s i +1 .
i =1Fig. 1. (a) INS results on E f = 2.4 meV. (b) INS results on E f = 3.0 meV.

By ﬁtting the calculated intensity to thetemperature difference obtained in the experiment using the least-squares method,
we estimated the optimum exchange andDM parameters. The obtained parameters
are bellow; J x = J y = −6.51 ± 0.04K,
z = 0.257 ± 0.10
J z = −5.43 ± 0.05 K, D1,2
z = D z = 0.284 ± 0.12 K. The
K, and D2,1
3,1
Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 929- 123 -

JAEA-Review 2013-039

1-2-48

Crystal Field Softeing and Magnetic Phase Transition in HoB4
T. Matsumura and D. Okuyama(B)
AdSM, Hiroshima University, RIKEN CMRG (B)A tetragonal rare-earth system of RB4
has attracted interest as a sytem where thequadrupolar and magnetic degrees of freedom are active on the so-called ShastrySutherland lattice.
HoB4 exhibits twophase transitions at TN1 = 7.5 K and at
TN2 = 5.9 K. The details of the magnetic structures and the anomalous natureof the phase transitions have been reported
in Ref. 1. Below TN1 an incommensurate
magnetic order sets in with Q=(δ, δ, δ ) (δ =0.022, δ = 0.07), followed by a ﬁrst ordertransition into a commensurate order with
Q=(1, 0, 0) at TN2 . One of the anomalous results in the study was the very broad magnetic diffuse scattering around (0, 0, 0.5)
and (1, 0, 0). In order to clarify the origin of
this diffuse scattering and the anomalous
phase transitions, we have carried out aninelastic neutron scattering experiment ona triple-axis spectrometer HER, using cold
neutrons to achieve high energy resolution
at low energies. Horizontal focusing analyzer, radial collimator, Be and PG ﬁlters
were used at an ﬁnal energy of 5.01 meV.
Fig. 1 shows the temperature dependences of the CEF excitation energy at
Q=(1, 0, 1) and (2, 0, 0.43). The former andthe latter corresponds to the commensurate
and incommensurate magnetic structures,
respectively. As shown by the plot, the CEF
energies at these Q-vectors decrease withdecreasing temperature down to TN1 . Simultaneously, in the paramagnetic phase
above TN1 , quasi-elastic peaks graduallydevelop at these Q-vectors. The temperature dependences of the inverse intensity are plotted in the bottom ﬁgure. This
clearly demonstrates that the commensurate and incommensurate correlations coexist in the paramagnetic phase, and wellfollow the Curie-Weiss behavior until they
diverge at the respective transition temperatures. This can be understood within themean-ﬁeld approximation.
The softening of the CEF can also be understood within the mean-ﬁeld approximation as reﬂecting χ( Q, ω ) = χ0 (ω )/(1 −J ( Q)χ0 (ω )). The CEF softening shows thatthe ground state of a Ho ion is a singlet
with no magnetic moment and that themagnetic order of HoB4 is caused by themixing with higher CEF states. It was clariﬁed that the diffuse scattering reported inRef. 1 was these CEF excitations reﬂectingJ ( Q ).
Therefore, at zero magnetic ﬁeld, there
seems no indication of a magnetic frustration effect caused by the ShastrySutherland type lattice.
(1) D. Okuyama et al., J. Phys. Soc. Jpn.,
77, 044709-1-14 (2008).

Fig. 1. (top) Temperature dependence of the 1st CEF
excitation energy of HoB4 at Q=(1, 0, 1) and (2, 0,0.43). (Bottom) Temperature dependence of the inverse intensity of the elastic peak at Q=(1, 0, 1) and(2, 0, 0.43).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 935- 124 -

JAEA-Review 2013-039

1-2-49Phase Transitions of Non-Kramers Pr Ions in a Trigonal Symmetry in Pr4 Ni3 Pb4
T. Onimaru1 , A. Ishida1 , K. Shigetoh1 , Y. F. Inoue1 , M. Nishi2 , T. J. Sato2 , Y. Oohara2 and
T. Takabatake1,3
1 AdSM, Hiroshima University, Higashi-Hiroshima 739-8530
2 Neutron Science Laboratory, ISSP, University of Tokyo, Tokai 319-1106
3 IAMR, Hiroshima University, Higashi-Hiroshima 739-8530
Multipolar degrees of freedom often play
an important role in 4 f electron systems.
Non-Kramers ions such as Pr3+ and Tm3+
possess multipolar degrees of freedom
other than magnetic dipoles even in a trigonal symmetry. In the present work, wehave focussed on a Pr-based intermetallic
compound Pr4 Ni3 Pb4 crystallizing in thetrigonal La4 Ni3 Pb4 -type structure (spacegroup R3) without inversion symmetry.[1,2] In the unit cell, Pr ions occupy the 3a and9b sites with the C3 and C1 point symmetries. In the C3 point symmetry, a nine-foldmultiplet 3 H4 splits into three Γ1 singlets
and three Γ23 doublets with quadrupolar
degrees of freedom. The isothermal magnetization shows a shoulder-like anomaly
at 4 T only for B||c, suggesting that an excited Γ23 doublet exists at a low energy of
4 K above the Γ1 singlet ground state. The
speciﬁc heat has cusp-type double anomalies at TN1 =2.7 K and TN2 =2.1 K which
are probably attributed to the Γ1 -Γ23 quasitriplet.
Neutron diffraction measurements on asingle crystalline sample were performed
using the ISSP High Q-resolution TripleAxis Spectrometer HQR(T1-1), in order todetect magnetic peaks below the transition
temperatures. Figure 1 shows the Q-scanalong the (1,0,L) line. A magnetic peak appears at Q=(1,0, 14 ) and its equivalent positions below TN2 =2.1 K. At the temperature range between TN2 and TN1 , the peakat (1,0, 14 ) splits into two peaks at (1,0, 14 ±δ)(δ∼0.1) where positions shift on cooling.
These behaviors indicate an incommensurate magnetic structure. We observed bothpeaks at 2.14 K close to TN2 , suggestingthat the IC-C transition at TN2 should be ofﬁrst order. Comparing the intensities of theequivalent magnetic peaks, they tend to bestrongly suppressed as the peak positions
approach to the [001]∗ direction. It meansthat the magnetic moments have a trend toalign along the c-axis in the ordered structures. Detailed analyses of the magnetic
structures are 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.

Fig. 1. Q-scan along the (1,0,L) line. The magnetic
10 14 peak appears below TN2 =2.1 K.

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JAEA-Review 2013-039

1-2-50Giant Uniaxial Anisotropy in the Magnetic and Transport Properties of CePd5 Al2
T. Onimaru1 , Y. F. Inoue1 , K. Ohoyama2 and T. Takabatake1,3
1 AdSM, Hiroshima University, Higashi-Hiroshima 739-8530
2 Institute for Materials Research, Tohoku University, Sendai 980-8577
3 IAMR, Hiroshima University, Higashi-Hiroshima 739-8530
CePd5 Al2 crystallizing in the tetragonal
ZrNi2 Al5 -type structure shows successive
antiferromagnetic orderings at TN1 =4.1 K
and TN2 =2.9 K.[1] The temperature dependence of resistivity ρ shows a Kondo metal
behavior with large anisotropy, ρc /ρ a =3.2
at 20 K, and opening of a superzone gap
along the tetragonal c-direction below TN1 .
The magnetic data of χ( T ) and M(B) in
the paramagnetic state were analyzed using a crystalline electric ﬁeld (CEF) model.
It led to a Kramers doublet ground statewithfunctions consisting primarily
 wave5
of ± 2 ,. The excited states are at 230 and
300 K. This CEF effect gives rise to thelarge anisotropy in the paramagnetic state.
In the ordered state, the uniaxial magnetic
anisotropy is manifested as Mc /Ma =20 in
B=5 T and at 1.9 K, and χc /χ a =25 in B=0.1
T and at 4 K.[2]In the present work, we performed powder neutron diffraction experiments using HERMES of IMR. Neutrons with a
λ=1.82646(6) Å were obtained by the 331
reﬂection of the Ge monochromator. Figure?? shows the powder neutron diffraction
patterns of CePd5 Al2 at various temperatures 1.4, 3.3 and 5.5 K. The patterns at 1.4
K and 3.3 K are vertically offset by 1000 and2000 counts, respectively, for clarity. At 5.5
K, all the peaks can be indexed as nuclear
Bragg peaks of the tetragonal ZrNi2 Al5 type structure. No secondary phase wasfound in the patterns being consistent with
the X-ray diffraction analysis. Although
the intensities of the nuclear peaks do notchange between 5.5 K and 1.4 K, weak superlattice peaks appear at 3.3 K and 1.4 K
at the scattering angles 2θ =8.1◦ and 21.7◦ ,which are shown with the thick arrows. On
cooling, the intensity starts to increase at 4
K, which is in good agreement with TN1 .

Thus the superlattice peaks originate in themagnetic transition at TN1 . The propagation vector of magnetic structures does notchange at TN2 , which hints to a possible
magnetic structure. From the analysis of
χ( T ), we propose canting of the magnetic
moments from the c-direction. Anothermodel is square-up of a modulated sinewave structure with appearance of higher
order reﬂections, because the magnetic entropy changes largely at TN2 as is found in
the speciﬁc heat. However, no higher order
reﬂections was observed in the present experiments. This is probably because the intensity was too weak to detect by means of
the powder neutron diffraction technique.
These results have already been publishedin ref. [2]. We plan to perform neutron
diffraction experiments on a single crystal
to determine the propagation vector.
References[1] R. A. Ribeiro et al.: J. Phys. Soc. Jpn. 76(2007) 123710.
[2] T. Onimaru et al.: J. Phys. Soc. Jpn. 77 (2008)
074708.

Fig. 1. Powder neutron diffraction patterns at T =1.4
K (T < TN2 ), 3.3 K (TN2 < T < TN1 ) and 5.5 K (T > TN1 ).

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1-2-51

Magnetic structure of Nd0.33Sr1.66MnO4
Y. Oohara, M. Kubota, and H. Kuwahara
ISSP, Univ. of Tokyo, PF, KEK Fac. Sci. & Tech, Sophia Univ.
Order of orbital state plays an importantrole in magnetic order of manganite compounds. The magnetic order of manganite consists of linear or zigzag ferromagnetic chain, which is inﬂuenced by orbital
order. In Nd1+xSr1-xMnO4 at x=3/4, thelinear ferromagnetic chain is established in
the magnetic ordered phase. On the other
hand, zigzag one is expected to exhibit at
x=2,/3. To see if it is appropriate or not, wehave performed neutron diffraction on the
crystal sample of x=2/3.
The neutron diffraction measurements
were performed with the ISSP triple-axis
spectrometer GPTAS and HQR installed atthe 4G and T11 experimental port JRR-3 in
JAEAI (Tokai).
Figure shows the (h 0 0) line scan at 13
K. The peak position is with
h=0.5, which is same position as the x=3/4
position, h=0.5.
The observed data suggests that the magnetic order does not consists of zigzag ferromagnetic chain. However, the order isshort-ranged.
It explaines why the crystal structure at
x=2/3 is tetragonal.

Fig. 1. Line scans along (h 0 0) at 13 K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-52Magnetic excitations in YbV4O8
Y. Oohara, M. Kubota, and Y. Kanke
ISSP, Univ. of Tokyo, PF, KEK and NIMS
YbV4O8 exhibits complex magnetic phasetransitions with charge order.
In the low temperature, we ﬁnd thatthe magnetic moments disappearfrom themagnetic susceptibility measurements. To
explore the mechanism of this disappearance, we have performed inelastic neutron
scattering measurements.
We prepared the 10cc powder sample.Neutron scattering measurements were
performed with ISSP
spectrometer HER and HQR installed at
C11 and T11 experimental ports at JRR3
(JAEA). The sample is cooled with closed
cycle refrigerator.
Figure shows the energy proﬁle at Q=1 A1 at 10 K.There is a peak at 2.5 meV. It
suggests that a spin-singlet is formed in
the low temperature with the 2.5 meV coupling, which disappear the magnetic moment observed in susceptibility measurements.

Fig. 1. Energy proﬁles at 1 A-1 at 10 K.

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1-2-53

Multiple temperature and ﬁeld induced phase transitions in new geometricfrustration material Co2(OH)3Br
M. Hagihalaˆ1, X.G. Zhengˆ1, Taku J Sato ˆ2
1. Saga Univ. 2. ISSP, Univ. of Tokyo
Co2(OH)3Br is a new geometrically frustrated compound in deformed pyrochlore
lattice. Previously we reported the coexistence of ferromagnetic order and spin
ﬂuctuation in Co2(OH)3Cl [1]. Later wefound its sister compound Co2(OH)3Br
is an antiferromagnetor with succssesivetransitions at TN1=6.2K and TN2=4.8K[2,3]. Recently we further found ﬁeldinduced multiple transitions under appliedmagnetic ﬁeld. The present study was designed to determine the zero-ﬁeld as wellas the ﬁeld-induced magnetic structures.
Elastic neutron scattering measurements
were performed at 4G:GPTAS using polycrystalline Co2(OD)3Br. Under zero ﬁeld,
we observed the antiferromagnetic reﬂections of k1=(0 -1/2 1/2) below TN1, andfurther another independent k2=(0 0 3/2)
below TN2. For the lower temperaturephase we have succeeded in determining
its magnetic structure, which is illustarted
in Fig. 1.
For the ﬁeld-induced phases, we observed a new antiferromagnetic order for
H > 6 kOe. At higher ﬁelds of H > 30
kOe a ferromagnetic order similar to thatin Co2(OH)3Cl appeared. Further work isin progress to determine all of the magnetic
structures.

Fig. 1. The magnetic structure for the low temperature antiferromagnetic order in Co2(OD)3Br

References[1] X. G. Zheng et al. Phys. Rev. Lett. 97(2006) 247204.
[2] M. Hagihala et al. J. Phys. : Cond. Matt.
19 (2007)145281.
[3] M. Hagihala, X.G. Zheng, T.
Kawae,Physica B 404 (2009)607.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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1-2-54

Neutron powder diﬀraction of TbPd3S4 in magnetic ﬁelds
E. Matsuoka(A), Y. Sasaki(A), T. Matsumura(B), K. Ohoyama(C), H. Onodera(A)(A)Department of Physics, Tohoku University, (B)ADSM, Hiroshima University, (C)Institutefor 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].
TbPd3S4 shows an antiferromagnetic(AFM) transition at TN=2.5 K. The neutron powder diffraction study of TbPd3S4
has revealed that the magnetic structure
below TN is described by a wave vectorof k = (100) [2]. TN shows an anomalous
magnetic-ﬁeld dependence. By applying amagnetic ﬁeld below 0.5 T, TN decreases
with increasing magnetic ﬁeld, while it
increases with increasing magnetic ﬁeld
above 0.5 T. The increase of TN above 0.5
T implies that the ﬁeld-induced antiferroquadrupolar (AFQ) ordering occurs above
0.5 T. To examine the possibility of ﬁeldinduced AFQ ordering, neutron powder
diffraction study of TbPd3S4 in magnetic
ﬁeld has been performed using HERMES
installed at the JRR-3M reactor in JAEA.
Neutrons with a wavelength of 1.8204(5) A
were obtained by the 331 reﬂection of the
Ge monochromator.
Fig. 1 shows the magnetic-ﬁeld dependence of the integrated intensities of 100
and 110 Bragg peaks measured at 1 K (T< TN). At zero magnetic ﬁeld, 100 and 110
are magnetic and nuclear Bragg peaks, respectively. The integrated intensity of 100
peak decreases gradually with increasing
magnetic ﬁeld, while that of 110 increase
by applying magnetic ﬁeld. Such ﬁeld dependence can be understood by considering the process that the AFM structure withwave vector of (100) is destroyed gradu-

ally by magnetic ﬁeld. At 0.5 T, the decrease rate of the integrated intensity of
100 and increase rate of that of 110 becomelarge abruptly, implying that the magnetic
structure changes from the (100)-type AFM
structure to a canted-AFM structure at 0.5
T. Similar canted-AFM structure has been
observed in DyPd3S4[3] and the appearance of such a canted structure is the evidence of a coexistence of AFM and AFQ
ordering in DyPd3S4 [3]. We therefore conclude that AFQ ordering is induced for
TbPd3S4 above 0.5 T.
[1] K. Abe et al., Phys. Rev. Lett. 83 (1999)
5366.
[2] E. Matsuoka et al., J. Magn. Magn.
Mater. 231 (2001) L23.
[3] L. Keller et al., Phys. Rev. B 70 (2004)
060407.

Fig. 1. Magnetic-ﬁeld dependence of the integrated
intensities of 100 and 110 Bragg peaks for TbPd3S4.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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1-2-55

Inelastic neutron scattering study on 1/1 approximant Ag-In-Tb
S. Ibuka, K. Matan and T. J. Sato
NSL, ISSP, University of 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. Quasicrystal can include magnetic ions, calledas ”magnetic quasicrystals”. These magnetic quasicrystals provide us an intriguing playground to experimentally investigate the magnetic ordering and dynamics
in the quasiperiodic spin systems.
Macroscopically, the magnetic quasicrystals mostly show the spin-glass-type freezing at low temperatures, as seen in the ZnMg-RE (RE: rare-earth) quasicrystals. Nevertheless, the spin dynamics, observed byneutron scattering, is very different fromcanonical spin-glasses; in several magnetic quasicrystals, highly localized inelastic mode was observed as broad inelastic
peak [1]. The origin of the inelastic mode
is inferred to be spin-wave-like modes localized in the dodecahedoral spin clusters, which are characteristic clusters in the
icosahedral quasicrystals. To conﬁrm thisidea, we have performed neutron inelastic
scattering study in the Ag-In-Tb 1/1 approximant, which is made of icosahedralclusters arranging periodically.
Polycrystalline
samplesofthe
Ag47 In39 Tb14 1/1 approximant wereprepared in usual manner. The powderedsample was loaded in the closed cycle 4 He
refrigerator, and the inelastic spectrum wasobserved using the ISSP-GPTAS and ISSPHER triple-axis spectrometers installed at
the JRR-3 research reactor.
Figure 1 shows the inelastic spectra atseveral temperature in the range of 3.5 <T < 150 K. In the high temperature range,
only the quasielastic response may be seenin the spectrum, whereas as the temperature is decreased, evolution of the low energy peak around 4 meV is evident. We
note that this behavior is almost the sameas those observed in the Zn-Mg-Tb quasicrystal (except for the characteristic energy scale), and thus conclude that theinelastic mode is due to the local highsymmetry clusters commonly found in thequasicrystalline and crystalline phases.
[1] T. J. Sato et al., Phys. Rev. B 73 (2006)
054417.

Fig. 1. Inelastic scattering spectrum of Ag-In-Tb. A
broad peak at 4 meV appears below 60 K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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1-2-56

Neutron scattering study on magnetic quasicrystal Zn-Mg-(Y,Gd)
S. Ibuka, K. Iida and T. J. Sato
NSL, ISSP, University of 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. Quasicrystal can include magnetic ions, calledas ”magnetic quasicrystals”. These magnetic quasicrystals provide us an intriguing playground to experimentally investigate the magnetic ordering and dynamics
in the quasiperiodic spin systems.
Macroscopically, the magnetic quasicrystals mostly show the spin-glass-type freezing at low temperatures, as seen in the ZnMg-RE (RE: rare-earth) quasicrystals. Nevertheless, the spin dynamics, observed byneutron scattering, is very different fromcanonical spin-glasses, and sometimes exhibits temperature independent S( Q, h̄ω )in the neutron scattering spectrum [1].
The temperature independent S( Q, h̄ω )is very unusual. One intriguing mechanism of the temperature independence isthe proximity to the quantum critical point(QCP) [2]. On the other hand, the temperature independence may be simply due to
distribution of the crystalline electric ﬁeld
(CEF) levels. To conclusively judge whichis the case for the magnetic quasicrystal, we
have performed neutron inelastic scattering experiment in the Zn-Mg-(Y,Gd) quasicrystal, where the half-ﬁlld 4f level of the
Gd3+ ions do not have CEF splitting inprinciple.
The neutron inelastic scattering study
was performed using the ISSP-GPTAS(4G)
and ISSP-HER(C11) triple-axis spectrometers installed at the JRR-3 research reactor. A powdered icosahedral sample ofthe composition Zn60 Mg30 Y8.5 160 Gd1.5 was
prepared in the usual manner. It may be
noted that to avoid the huge neutron absorption of natural Gd, we used the stable
isotope.
Figure 1 shows the resulting inelastic

scattering spectra at several temperatures
spanning 1.4 K to 50 K, observed using the ISSP-HER spectrometer with theoutgoing neutron energy of 2.75 meV. It
is clearly seen that the spectrum for theneutron-energy-loss side exhibits almost
temperature-independent behavior. Thisbehavior is indeed exactly the same as what
has been observed in the Zn-Mg-Ho quasicrystal. Therefore, we can conclude thatthe origin of the temperature independence
is not due to the accidental distribution of
the CEF levels. Instead, a closer relation to
the QCP mechanism is highly suggested.
[1] T. J. Sato et al., Philos. Mag 87 (2007)2939.
[2] M. C. Aronson et al., Phys. Rev. Lett.
75 (1995) 725.

Fig. 1.
(Y,Gd)

Inelastic scattering spectrum of Zn-Mg-

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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1-2-57

Magnetic structures in magnetic ﬁelds of TmB4 with the Shastry-Sutherland
lattice
Iga F. (a) , Michimura S. (a), Matsumura T. (a), Takabatake T. (a), Ohoyama K. (b)(a) ADSM, Hiroshima Univ., Higashi-Hiroshima, Hiroshimna 739-8530, Japan (b)IMR,
Tohoku University, Katahira, Sendai 980-8577, Japan
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) [1]
where nearest-neighboring dimers geometrically frustrated.
Our previous study of powder neutron diffraction in TmB4 shows incommensurate antiferromagnetic (IC AFM)
andorderings at 11.7 K and 10.7K,
incommensurate-commensurate(IC-C)
transition at 10 K [2]. From the magnetic
phase diagram as shown in Fig.1, phase IV
shows a simple antiferromagnetic patternwith a propagation vector of k4=(1, 0,0). The Phase III has been assigned withpropagation vector k4 and an additional
long period modulation vector k3=(0.13,0, 0). Furthermore, the phase II was also
indexed with the k4 and k2=(0.012, 0.012,
0) and k2 =(0.036, 0.012, 0). We have foundthat TmB4 shows a multi-step magnetization process. The magnetization for B//cshows not only a 1/2 Ms plateau in phase
VI as in RB4 (R=Dy, Ho, Er, Tb) but also a
1/8 Ms plateau in phase V [3]. Here, Msmeans the saturation moment of Tm3+ ion.
In order to clarify these ordering vectors inthese magnetic phases, we have performed
neutron diffraction experiment on a single
crystal sample of Tm11B4.
High-quality single crystal sample of
TmB4 was grown by ﬂoating zone method
using a four-xenon lamps image furnace.
The neutron diffraction experiment inﬁelds up to 6 T was performed in the
triple axis spectrometer, TOPAN (6G).
The incident neutron energy Ei was tuned
to 30.5 meV (1.64 A). The sample wasplaced with the (h k 0) plane in order to set

parallel to the neutron scattering plane inﬁeld applied along [001] axis.
From the neutron diffraction in magnetic
ﬁelds, the incommensurate and commensurate magnetic structures based on the 8unit cell period were found in the Plateau
phase (V, VI). The magnetic structure ordered in the ﬁeld accompanied by the magnetic plateau has a similar value as the period determined in phase III with magnetic
ﬂuctuation. Frustration on the SSL plays
an important role to form the magnetic
plateaus. The super-lattice reﬂections without magnetic origin were found in the 4unit cell period for a-axis in the phase V.
This suggests that the periodic magnetic
structure with 8-unit cell period locks into
the period crystal lattice.
References[1] B. S. Shastry and B. Sutherland, Physica
B & C 108B (1981), p. 1069.
[2] S. Michimura et al., J. Phys. Soc. Jpn. 78(2009), 024707.
[3] F. Iga et al., J. Magn. Magn. Mater. 310(2007) e45-47.

Fig. 1. Fig. 1 Magnetic phase diagram of TmB4.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-58Magnetic State in the Tm-based Reentrant Superconductor Investigated by the
Powder Neutron Scattering
N. Kase1 , Y. Tomiyasu2 , T. Muranaka1 , and J. Akimitsu1
1 Department of Physics and Mathematics, Aoyama-Gakuin Univ., 5-10-1 Fuchinobe, 2

Department of Physics, Tohoku Univ., 6-3 Aoba, Sendai, 980-8578
The Tm-based reentrant superconductor Tm5 Rh6 Sn18 exhibits superconductivity at Tc = 2.2 K[1] and reentrant behavior between 1.0 and 1.45 kOe[2]. From themuon-spin rotation/relaxation (μSR) measurements, we reveal the coexistence between magnetism and superconductivity
under a zero magnetic ﬁeld, and a development of magnetic ordering is observed
below around 10 K[3]. However, the magnetic ordering cannot be described as a simple long-range magnetic ordering.
To understand magnetic state more precisely, magnetic structure of Tm5 Rh6 Sn18
has been investigated by a powder neutron
scattering as shown in Figure 1, which represents the neutron powder diffraction pattern at 0.75 K and 10 K. We could not observe any Bragg peak due to a long-range
magnetic order in any temperature region
and also observe a magnetic diffuse scattering attributed to a short-range order inthe low-angle region below 10 K. The diffuse scattering intensity can be described
as a conventional Gaussian function. Furthermore, the temperature dependence of
the integrated intensity is almost consistent with the results of muon precession
frequency obtained from the ZF-μSR measurement.
Therefore, we conclude that the magnetic order can be considered not to be longrange ordered but superparamagnetic; ferromagnetically ordered within a certain
cluster, but, paramagnetically ﬂuctuating
between the cluster, and the superparamagnetic cluster gradually develops below
around 8 K. The size of the magnetic cluster is so large that a spontaneous oscillation signal is clearly observed from ZF-μSR
measurement. This scenario makes it pos-sible to explain the occurrence of the reentrant superconductivity; the ﬁeld-induced
magnetic order obtained from the electricalresistivity measurements under magnetic
ﬁelds is originated from an alignment ofeach spin of magnetic clusters to the same
direction. Thus, superconductivity is not
destroyed under zero magnetic ﬁled below
Tc .
References[1] J. P. Remeika et al.: Solid. State. Commun.
34 (1980) 923.
[2] A. Rojek et al.: Phys C 223 (1994) 111.
[3] N. Kase et al.: to be submitted in J. Phys.
Soc. Jpn..

Fig. 1. The neutron powder diffraction pattern at
0.75 K and 10 K of Tm5 Rh6 Sn18 . The inset showsthe expansion of the low-angle region.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-59Neutron diﬀraction experiment under high pressure in YbMn2 Ge2
T. Fujiwara A , N. AsoB , M. NishiC , Y. UwatokoD
A Yamaguchi Univ., B Univ. Ryukyus, B ISSP Univ. Tokyo, C ISSP-NSL Univ. Tokyo

YbMn2 Ge2 with ThCr2 Si2 type bodycentered tetragonal structure is an intermediate valence system and its magnetic
property is dominated by magnetic exchange interactions between Mn moments.
This system shows a quite unique magnetism in which two antiferromagnetic
states, AFM I at TN2 < T ≤ TN1 ≈ 405 K
and AFM II at T ≤ TN2 = 163 K, competewith each other. With applying hydrostaticpressure, the system indicates valence transition of Yb ions at Pc ∼ 1.25 GPa. Althogh,
magnetic behaviors of the system drastically change above Pc and new magnetic
phases, AFM III and IV, induced upon pressurization, the details of magnetic structures in AFM III and IV states are not clariﬁed yet. In this work, we have carried out
the neutron diffraction experiment within
the reciprocal lattice plane (HHL) of single crystal YbMn2 Ge2 under high pressureusing a clamping-type high pressure cellmade of hardened Cu-Be alloy.
Figure 1 is rocking curves at Q = (111) in
YbMn2 Ge2 under P = 1.3 GPa at T = 8 K
and 300 K. As shown in the ﬁgure, magnetic bragg peak is clearly observed in both
AFM III (300 K) and AFM IV (8 K) states.
This indicates an existence of antiferromagentic component consists of that a ferromagnetic (00) Mn planes couples antiferromagentically along [001] direction. It is
recognizable that an increase of (111) peakintensity occurs simultaneously when thesystem undergoes a magnetic phase transition from AFM III to IV with decreasing temperature under 1.3 GPa. Unfortunately, we could not observe any magnetic
bragg reﬂection under P = 1.3 GPa except(111) and (113). Therefore, it is necessary
to perform the similar neutron diffraction
experiments on (H0L) and (HK0) reciprocal lattice planes under high pressure to obtain the detail information of the magnetic

structures in AFM III and IV states.

Fig. 1. Rocking curves at Q = (111) in YbMn2 Ge2under P = 1.3 GPa in AFM III (T = 300 K) and AFM
IV (T = 8 K) states.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-60Magnetic excitation in Co4B6O13
Masuda T., Hondo S. and Matsuura M.
Yokohama City University, Osaka University
Recently spin liquid in triangular lattice, Kagome lattice, Pyrochlore lattice,
etc has been attracted much attention.
Amongt them regular tetrahedron spin
system, Co4B6O13, was discovered recently[1]. Co2+ (S=3/2) ions are on the corner of tetrahedron. Since the Co-Co intratetrahdron distance 3.25 A is shorter than
the intertetrahedron 4.26 A this compoundis expected to be an isolated tetrahedronspin system. The magnetic susceptibility
shows broad maximum at T = 14 K and
it decreases drastically at low temperature.
No magnetic order is identiﬁed at T > 1.8
K. These are typical behaviors of spin gap
system with nonmagnetic ground state. In
the magnetization measurement an drastic increase was identiﬁed at H = 10 T and
multistep anomalies were observed at 40
T and 60 T. These anomalies are supposed
to be transition between eigenstates ofHeisenberg antiferromagnetic tetrahedroncluster, S=0 (quartet), S=1 (ninefold multiplet), S=2 (elevenfold multiplet). However,in quantitative level, the data cannot be
reproduced and additional terms such as
Dzyaloshinskii-Moriya interaction and single ion snisotropy would be required. Even
though rather complex, the isolated tetrahedron spin cluster is a rare experimental realization of exact solvable model withspin frustration. Hence to reveal the spin
excitation of Co4B6O13 we performed inelastic neutron scattering experiments.
Powder sample was obtained by hydrothermal synthesis. As a starting material we used 11B oxide to reduce the absorption of neutron. Orange type cryostat was used to achieve low temperature. Inelastic neutron scattering experiment was performed at C1-1 beamline. The
collimation setup is Guide-PG-40’-radialcollimation-Be ﬁlter-Horizontally focused
analyzer-open with Ef = 3 meV.

In Fig. 1 we show energy scan at q=1A1. Well dﬁned peaks are observed at hw= 0.96, 1.18, 1.61, 2.44, 2.92, 4.15, and 4.66
meV. These peaks are identiﬁed dispersionless in similar scans at different q. With
the increase of temperature the intensity
decreases. These results measn that thepeaks are of a magnetic cluster. The ﬁnepeak structure measn that the degenerated
eigenstate of a Heisenberg cluster is splitted by peturbative terms as magnetic susceptibility and heat capacity data indicated.
Q scans were also performed at several energies. The detailed data analysis is now
under progress. The summary of this study
will be published with additional nutron
scattering experiment somewhere.
[1] H. Hagiwara et al., fall meeting of Japan
Physical Socity, 20aQH (2008).

Fig. 1. Energy scan of Co4B6O13 at Q = 1A-1.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-2-61Degree of frustration in geometrically frustrated magnets (Co1-xZnx)Cr2O4
Tomiyasu K.(A), Yokobori T.(B), Horigane K.(C), Akimitsu J.(B), Yamada K.(C)(A)Dep. of Physics Tohoku Univ., (B) Dep. of Physics Aoyama Gakuin, (C)WPI-AIMR Tohoku
Univ.
frustration. In addition, even at x=0.90 thepeak positions of diffuse scattering are different from those of magnetic Bragg reﬂections in ZnCr2O4, suggesting that the spiral short-range order still survives.
1200
1100
1000
900

Counts / 77 mnt (~1 min) / 1 g

Highly frustrated systems, spinel
antiferromagnets ACr2O4 (nonmagnetic
A=Mg,Zn,Cd and Hg) consisting of acorner-sharing tetrahedron lattice as B (Cr)sites, are well-known to exhibit the phenomenon of spin hexamer on the kagome
plane. On the other hand, it was recently
reported that geometric frustration still
survives in spinel ferrimagnets ACr2O4(magnetic A=Co and Mn) as explained below. In these materials a spin forms a conical structure resolved into an Ising-typeferrimagnetic component and an incommensurate spiral one. As the temperature
decreases, although the former component
forms long-range order at T C=93 and 51
K, the latter one mainly starts to grow at
T S=25 and 14 K and does not achieve longrange order even in the lowest temperature phase. Therefore, it was proposed thatthe geometric frustration among the B-site
spins can coexist with the A-site spins, andis mainly reﬂected on the spiral component.
However, the spiral type seems to be
too different from the hexamer. Here, inorder to validate the expanded concept ofgeometric frustration, we report the spiralspin correlations of solid solution materials (Co1-xZnx)Cr2O4 by powder neutron
diffraction (x=0 to 1).
Figure shows the diffraction patterns
measured at elastic condition in the lowest temperature phases. The intensity of
111 fundamental reﬂection decreases withincreasing x from 0 to 0.45, then is almost constant, meaning that the ferrimagnetic component disappears. The magnetic
satellite reﬂections monotonically become
broad, most likely validating that the correlation length of spiral order corresponds
to the degree of expanded frustration, andthe spiral short-range order comes from the

800

111

Diffraction patternsof (Co1-xZnx)Cr2O4

x=0.00x=0.15x=0.30x=0.45x=0.60x=0.75x=0.90x=1.00

220

700
600
500
400
300
200
100
0
0.5

1.0

1.5

2.0

2.5

-1

Wavenumber [A ]Fig. 1. Figure. Elastic scattering data of (Co1xZnx)Cr2O4 in lowest temperature phases.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 994- 137 -

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JAEA-Review 2013-039

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1.  ୰ ᛶᏊᩓ஘ 3 ᙉ┦㛵㟁Ꮚ⣔

1. Neutron Scattering

3 Strongly Correlated Electron     
Systems- 139 -

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JAEA-Review 2013-039

1-3-1

Competition of diﬀerent antiferromagnetic correlations in a heavy fermion
Ce(Ru1-xRhx)2(Si1-yGey)2
Y. Tabata(A), S. Ohya(B), H. Taguchi(A), C. Kanadani(C), T. Taniguchi(B), H.
Nakamura(A)(A) Graduate School of Engineering, Kyoto University, (B) Graduate School of Science, Osaka
University, (C) RCMI, Toho University

Figure. 1 shows the xy phase diagram ofCe(Ru1-xRhx)2(Si1-yGey)2 obtained fromneutron scatteing experiments and magnetization measurements. A 3rd AFM phase
where both the q1and the q3 magnetic
scattering are observed, q1+q3-phase, hasben discovered between the q1- and theq3-phases. No hysteretic behavior was observed in the q1+q3-phase, and hence, we
conclude that the q1+q3-phase is a thermodynamic equilibrium state, may has adouble-q structure. And also, we havefound that the AFM phase appeared bysubstituting Ge for Si in CeRu2Si2 is not a
simple q1-phase but the q1+q3-phase.

097204 (2004).
[2] S. Kawarazaki et al., J. Phys. Soc. Jpn. 66,
2473 (1997).
[3] S. Dakin et al., J. Magn. Magn. Mater.
108, 117 (1992)., S. Quezel et al., J. Magn.
Magn. Mater. 76&77, 403 (1988).

0.35

Ce(Ru1-xRhx)2(Si1-yGey)20.30
Ge-concentration, yCeRu2Si2 is a paramagnetic heavy fermion
locating close to an antiferromagnetic(AFM) quantum critical point (QCP).
Interestingly, in this compound three
AFM correlations with the magnetic wave
vector q1=(0.31,0,0), q2=(0.31,0.31,0) and
q3=(0,0,0.35) coexist [1], and may competeeach other. By substituting Rh for Ru, theq3-AFM correlation develops the longrange magnetic order, q3-phase, in the
Rh-concentraion x range of 0.03 < x < 0.35
[2]. On the other hand, appearance of the
q1-AFM order, q1-phase, was reported
by substituting Ge for Si or by substituting La for Ce [3]. It takes a great interest in quantum phase transitions amongsuch a competing antiferromagnetic phases
and paramagnetic Fermi liquid (FL). As aﬁrst step for studying such quantum phasetransitions, we have grown many single
crystalline samples of Ce(Ru1-xRhx)2(Si1yGey)2 and have tried to make up the xy
phase diagram.

q1-phase

0.25
0.20

se?
pha
q 3+
q1

0.15
0.10

q3-phase
0.05

para.

0.00
0.00

0.01 0.02 0.03 0.04
Rh-concentration, x

0.05

Fig. 1. The xy phase diagram of Ce(Ru1-xRhx)2(Si1yGey)2 at T = 1.5K obtained from neutron scatteingexperiments. Asterisk, closed square, closed circle
and open circle denote the paramagnetic FL, the q1-,
the q3- and the q1+q3-phases respectively.

[1] H. Kadowaki et al., Phys. Rev. Lett. 92,
Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 603- 141 -

JAEA-Review 2013-039

1-3-2

Magnetic phase diagram under low temperature and high pressure in RVO3 II
D. Bizen(A), H. Nakao(A), K. Iwasa(A), Y. Murakami(A), T. Osakabe(B), S.
Miyasaka(C), Y. Tokura(D,E,F)(A) Tohoku Univ., (B) JAEA, (C) Osaka Univ., (D) The Univ. of Tokyo, (E) ERATO-MF, (F)
RIKEN-CMRG

In order to determine the magnetic ordering phase, the magnetic scattering was
explored by using the triple-axis spectrometer TOPAN. The temperature dependence of the magnetic peak intensities was measured at several pressures asshown in the ﬁgure. At ambient pressure(0GPa), the (0 1 0) magnetic peak reﬂecting the C-type spin ordering (C-SO) was
observed below TSO1=118K. Moreover, thesecond magnetic transition was observed
at TSO2=77K: there the magnetic peak at (01 0) disappears and that at (0 1 1) reﬂecting
the G-type spin ordering (G-SO) appears.

With increasing pressure, TSO2 remarkably
increases while TSO1 has few pressure dependence. As a result, the C-SO phase completely disappears above 3GPa. Furthermore, TSO2 continues to increase even after
the disappearance of C-SO phase. Finally,
we could elucidate that the magnetic transition at TSO2 just corresponds to OD/COO phase transition above 6GPa; such asimultanious transition has never been reported in perovskite-type transition metaloxides. The result indicates that the magnetic ordering play an important role for
the OD/C-OO phase transition.
[1] S. Miyasaka et al., Phys. Rev. B 68 (2003)
100406.
[2] D. Bizen et al., Phys. Rev. B 78 (2008)
224104; D. Bizen et al., J. Magn. Magn.
Mater. 310 (2007) 785.

Intensity (cnt./2000kMon.)

Perovskite vanadium oxide RVO3 (R: rearearth or Y) shows various physical properties coupled with the spin and orbital
states. [1] The orbital ordering is strongly
coupled with the lattice distortion, i.e.
Jahn-Teller distortion. Hence the pressure
effect for the orbital state interests us, andthe pressure-temperature phase diagramof the V 3d-orbital state was investigatedby x-ray diffraction under high-pressure
and low-temperature. [2] Under high pressure (> 6 GPa), the orbital disorder (OD)
- C-type orbital ordering (C-OO) phasetransition was newly found in YVO3. At
this transition, the space group does notchange, although the symmetry is usuallybroken at an orbital order-disorder transition. Such an orbital order-disorder phasetransition without the change of the spacegroup was actually reported in LaMnO3.
On the other hand, the magnetic symmetry breaking upon this phase transition canbe also expected. To make clear the relation between the spin and orbital states, wehave investigated the magnetic phase diagram of YVO3 under high-pressure andlow-temperature using a hybrid anvil cell.

0 GPa (×0.33)
1.0 GPa
3.0 GPa
4.9 GPa
6.2 GPa

800 (a)700 YVO3
600
500
400
300
200
100 B. G.
01200 (b)
1000
800
600
400
200
B. G.
0
60

TSO1

(010)
0 GPa (×0.22)
1.0 GPa
3.0 GPa
4.9 GPa
6.2 GPa

TSO2
80

(011)
100
120
Temperature (K)

140

160

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

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 690- 142 -

JAEA-Review 2013-039

1-3-3

Magnetic-Field Variations of Antiferromagnetic Structure in CeRh1-xCoxIn5
M. Yokoyama(A), Y. Ikeda(B), I. Kawasaki(B), D. Nishikawa(B), K. Tenya(C), H.
Amitsuka(B)(A)Ibaraki University, (B)Hokkaido University, (C)Shinshu Universitythat the properties of the Fermi surfaces
signiﬁcantly vary by Co concentrations.
[1] W. Bao et al., Phys. Rev. B 62 (2000)
R14621.
[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] M. Yokoyama et al., Phys. Rev. B 77
(2008) 224501.
[5] S. Ohira-Kawamura et al., Phys. Rev. B
76 (2007) 132507.

Intensity (arb. units)

The Ce-based heavy-fermion compounds
CeMIn5 (M=Rh and Co: HoCoGa5-type
tetragonal structure) are intensively studied for a rich variety of low-temperature
properties ascribed to the interplay of antiferromagnetism (AF) and superconductivity (SC). CeRhIn5 orders in an incommensurate AF phase with a modulation of qh =(1/2, 1/2, 0.297)[1]. It is revealed in the Codoped alloys CeRh1 − xCoxIn5 [2] that the
AF phase is suppressed with increasing x,
and then disappears at x c ˜ 0.7. At the sametime, SC appears between x = 0.4 and x = 1.
Recent our elastic neutron scattering (ENS)
measurements revealed the emergence ofa new AF state with modulations of qc1 =(1/2, 1/2, 1/2) in the intermediate x range,
followed by the suppression of the qh-AF
state[3-5]. To elucidate magnetic instability involved in small and intermediate x
ranges, we have further performed the ENS
experiment under magnetic ﬁeld for CeRh1− xCoxIn5.
Single crystals of CeRh1 − xCoxIn5 weregrown by the In-ﬂux method. The samples
were shaped into bar (typical size: ˜3 mmˆ2
× 10 mm) in order to minimize the effectsof the neutron absorption caused by Rh and
In. The ENS experiments were carried out
using triple-axis spectrometers GPTAS and
PONTA at the JRR-3M research reactor of
JAEA. Magnetic ﬁeld was applied along
the [110] direction, which are orthogonal
to the (hhl) scattering plane selected in thepresent study.
Figure 1 shows the neutron scattering pattern obtained from the (1/2, 1/2, L) scan at
1.6 K. It is found that applying ﬁeld along[110] switches the AF propagation vector
from qh to qc2 = (1/2, 1/2, 1/4) at x =0.23, while it integrates the qc1- and q1-AF
components [q1=(1/2,1/2,0.42)] into a single qc1 one at x = 0.7. This result suggests

140

CeRh Co In

120

Q=(1/2,1/2,1+ζ)B || [110]T=1.6 K

100
80

1-x

x

5

0T
3T

(b) x=0.7(a) x=0.23

60
40
20
0
-20
0.5 0.6 0.7 0.8 0.9

1 0 0.2 0.4 0.6 0.8
ζ (r.l.u.)

1

Fig. 1. The AF Bragg-peak proﬁles at B = 0 and 3 T
for CeRh1 − xCoxIn5 with (a) x = 0.23 and (b) 0.7.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 691- 143 -

JAEA-Review 2013-039

1-3-4

Magnetic Excitations of LaFeAsO0.89F0.11
Taketo Moyoshi, San Chul Lee, Ayaka Kawabata, Yoshiaki Kobayashi, Yukio Yasui,
Masatoshi Sato and Kazuhisa Kakurai1
Department of Physics, Nagoya University, Chikusa-ku, Nagoya 464-8602, 1 Quantum Beam
Science Directorate, JAEA, Tokai, Ibaraki 319-1195
This project was originally planned to
study the dynamical magnetic propertiesof honeycomb systems of Na3Cu2SbO6andNa2Co2TeO6 to investigate in detail theunusual behavior such as the spin gap phenomena found in the former one. However,
the machine time was used to measure themagnetic excitation spectra of newly foundsuperconducting system LaFeAsO1-xFx1)
to quickly obtain information on its electronic state useful to investigate the superconducting mechanism.
In LaFeAsO1-xFx, the superconducting
phase is derived by the F-doping to themagnetically ordered phase, and the highest transition temperature Tc is ˜ 28 K at
x˜0.11. Because the magnetic ﬂuctuation isconsidered to play a possible role in realizing the superconductivity, to study themagnetic excitation spectra of the system
one of the most important things for the
study of the superconducting mechanism.
The measurements were carried out for a
powder sample of LaFeAsO1-xFx (x˜0.11)
with the incident (Ei) or scattered (Ef) neutron energy being ﬁxed at 30.5meV. In themeasurements, the horizontal collimations
were 40 -40 -80 -80 . Scanning the absolute scattering vector Q at various ﬁxed
transfer energies E, we found a peak at Q
˜1.1 -1 corresponding to (?, 0) point in
the reciprocal space. Because the peak gets
sharper with decreasing T, they are considered to be magnetic. The integrated intensities Iint of the peaks have been estimated,
and in the ﬁgure, Iint/(n+1) (n: Bose factor) are shown against E at T = 3.5 K (<Tc) and 40 K (> Tc).These results should
be compared with the so-called resonancepeak, the existence of which is discussed
by Maier and Scalapino for the s? symmetry of the superconducting order param-

eter ?.2) Because the expected resonancepeak is expected to be very sharp, if itexists, the widths of the peaks of the ?
(Q,?)-? curve obtained with constant Ei,
for which the energy resolution widths are?3.3 meV, should be sharper than thoseobtained with constant Ef (the resolution
widths ?5.2 meV. As can be found in theﬁgure, we do not see appreciable changeof the curves with changing the experimental resolution, which suggests that theresonance peak does not exist. Recently,
the neutron scattering measurements onaligned crystals of BaFe1.84Co0.14As23)
and BaFe1.9Ni0.1As24) were reported. The
present data seems to be very similar tothat of BaFe1.9Ni0.1As2. Here, we note thatour data are consistent with the fact that
the Co doping effect on Tc of LaFeAsO1xFx (x˜0.11) is much weaker than expected
for the s? symmetry ﬁrst reported by us.5)
1)Y. Kamihara et al., J. Am. Chem. Soc. 130(2008) 3296.
2)T. A. Maier and D. J. Scalapino, Phys. Rev.
B 78 (2008) 020514.
3)M. D. Lumsden et al., arXiv: 0811.4755.
4)S. Chi et al., arXiv:0812.1354
5)A. Kawabata et al., Proc. Int. Symposium on Fe-oxipnikutide Superconductors,
June28-29, 2009, Tokyo and also J Phys. Soc.
Jpn., 77 (2008) 103704.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 718- 144 -

JAEA-Review 2013-039

1-3-5

Magnetic excitations of NaxCoO2.yD2O
Taketo Moyoshi, Yukio Yasui, Masatoshi Sato and Kazuhisa Kakurai1
Nagoya Univ. 1JAEA
Na0.3CoO2.1.3H2O with the triangular lattice of Co atoms exhibits the superconducting transition at Tc of 4.5 K.1) It attracted much attention as the oxide superconductor with 3d-electrons found after thehigh-Tc Cu-oxides, and various experimental and theoretical studies have been carried out to identify the superconducting
mechanism.
We have carried out the neutron magnetic
inelastic scattering to investigate the relationship between the magnetism and thesuperconductivity. We used aligned crystals of NaxCoO2.yD2O, in which the volume fraction of the superconducting phaseor the one with y˜1.3 was about 75%.
The remaining non-superconducting phase
was found not to contain D2O. On thisaligned sample, we have carried out measurements three times. During the periods (nine months) between these experiments, the sample was kept in the He
gas with D2O vapor. The c-axis lengthof the superconducting phase was deterand
mined to be 19.7038(7) , 19.706(2)19.653(2) just before the ﬁrst, second andthird experiments, respectively. This indicates that the deuterated parts of the crystals are at the boundary between the lowernuQ3 superconducting and nonsuperconducting regions in the Tc-nuQ3 phase diagram shown in ref. 2 at the ﬁrst and second experiments and at middle point of
the lower-nuQ3 superconducting phase at
the third experiment. (nuQ3˜3nu,nuQ being the NMR quadrupolar frequency.)
Scans of the transfer momentum Q along(h, 0, 2.8) in the reciprocal space with ﬁxed
transfer energy (E) have been carried out
at E= 3 meV at several temperatures between 5 K and 100 K. In all experiments,
two magnetic scattering peaks have been
observed at h˜0 and h˜1/2. The peak at h˜0corresponds to an in-plane ferromagnetic

ﬂuctuation and the peak at h = 1/2 corresponds to the in-plane antiferromagnetic
ﬂuctuation.
We ﬁnd that the Q-integrated intensity kai(omega= 3 meV) estimated for the peak observed at h ˜ 0 decreases with decreasing T
and becomes inappreciable at low temperature, while kai (omega= 3 meV) at h = 1/2
exists at all temperatures studied here. The
disappearance of kai (omega= 3 meV) ath˜0 at low T excludes the existence of thehole pockets near the K points in the reciprocal space. We do not show the detailed
reasons here, but just mention that the existence of the peak in a relatively high T region is due to the fact that the top of theeg band is slightly below the Fermi level.3)
Important point is that this result excludes
the basis of the predicted triplet superconductivity.4) The incommensurate magnetic
ﬂuctuations with a small wave vector q (orh˜0) suggested by Kuroki et al.5) as the excitations among the electron levels of two
different Fermi surfaces around the gamma
point, are also excluded by the disappearance of the scattering peak at h˜0. The resulton the Fermi surface topology is consistent
with the simple Fermi surface observedby the angle-resolved photoemission spectroscopy (ARPES) reported by Shimojima
et al.6)
The two-dimensional antiferromagnetic
ﬂuctuations have been observed in the Q
region around (1/2, 0, l). This result indicates that, if spin ﬂuctuations are important
for the occurrence of the superconductivity,
they should be antiferromagnetic, supporting singlet pairing.
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.7)

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 740- 145 -

JAEA-Review 2013-039

1) K. Takada et al.: Nature 422 (2003) 53.
2) Y. Kobayashi et al.: J. Phys. Soc. Jpn. 76(2007) 103705.
3) K. Yada and H. Kontani: J. Phys. Soc. Jpn.
74 (2005) 2161.
4) Y. Yanase et al.: J. Phys. Soc. Jpn. 74 (2005)
430.
5) K. Kuroki et al.: Phys. Rev. B 73 (2006)
184503.
6) T. Shimojima et al.: Phys. Rev. Lett. 97(2006) 267003.
7) Y. Kobayashi et al.: J. Phys. Soc. Jpn. 77(2008) 063703.

1-3-5- 146 -

JAEA-Review 2013-039

1-3-6

Fe-doping dependence of magnetic correlations in Bi2201
H. Hiraka and K. Yamada
IMR, Tohoku University, AIMR, Tohoku University
with large δ detected by Fe doping may
come from underlying modulations of Cu
spins. The large δ of the current sample in the ocerdoped phase follows a relation δ = p, where p is the effective holeconcentration and estimated to ∼0.22 from
ARPES measurements for y = 0.09 [2]. Thisstrongly suggests a different type of spincorrelations in Bi2201 from the dominant
spin-stripe correlations in Sr-doped La214.
References[1] H. Hiraka and K. Yamada, Activity Reporton Neutron Scattering Research: Experimental Reports 15 (2008), Report Number
398.
[2] T. Sato, private communications.
Bi1.75Pb0.35Sr1.90Cu1-yFeyO6+δ, as-grown
AKANE, Ge(311)M+PG(002)A, Unpolarized, 20Ei
y = 0.12
0.06
0.03

600

Net counts, I3K - I70K / ~12 min

To explain the origin of high-Tc superconductivity, it is important to investigate spin correlations in a wide carrierconcentration range for high-Tc cuprates
systematically.
Although no magnetic
cross section has been experimentally reported yet in one of the most typicalcuprate superconductors Bi2201, we succeeded in ﬁnding magnetic incommensurate peaks at quasi-elastic channel by using a Fe and Pb co-doped single crystal
on AKANE last year [1]. The most striking feature of the magnetic scattering is
the anomalously large incommensurability δ = 0.20. Since δ in Sr-doped La214
system saturates in 0.13 ∼1/8, it should
be examined ﬁrst whether the large δ in
Fe-doped Bi2201 come from the underlying Cu-spin modulation or merely the
Fe-Fe magnetic interaction between localized spins. So, we searched the Fe-doping
dependence of the magnetic incommensurate peaks using as-grown single crystals of Bi1.75 Pb0.35 Sr1.90 Cu1−y Fey O6+δ with
y =0.03, 0.06, and 0.12. To compare
the scattering intensity each other, samples
with nearly the same sample volume wereprepared for current studies.
Neutron scattering experiments werecarried out on triple-axis spectrometers
AKANE and TOPAN. Figure 1 shows difference plots of Q spectra between 3 K
and 70 K about (1, 0, 0) antiferromagnetic
zone center. While the magnetic intensity successively increases upon Fe doping, the incommensurate-peak structure isunchanged within the statistics. In fact,
the spectra are well reproduced by using the same incommensurability and peakwidth, already extracted from y = 0.09 [1].
This result could be explained by supposing small magnetized clusters around Fe,
which grow in number with increasing Fe
spins. Hence, the magnetic modulations

400

200

0

-0.5

0

0.5

(1+ζ, ζ, 0)

Fig. 1. Difference plots of Q spectra of Fe-doped
samples for Fe-doped Bi2201 with y = 0.03, 0.06,
and 0.12. The curved lines are ﬁts to a pair ofLorentzians by holding the peak position and thepeak width ﬁxed.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 761- 147 -

JAEA-Review 2013-039

1-3-7

Identiﬁcation of an order parameter in a heavy fermion antiferromagnet CeTe3
K. Deguchi1 , N. Aso2 , 3, H. Iwase1 , T. Okada1 , G. F. Chen1 , N. K. Sato1 , H. Yoshizawa3
Nagoya Univ.1 , Univ. of the Ryukyu2 , NSL-ISSP, Univ. of Tokyo, Graduate School of Sci.3
Rare-earth tri-telluride CeTe3 , which belongs to the family of quasi-two dimensional compounds RTe3 (where R = Y, LaSm, Gd-Tm), has highly two-dimensional
crystal structure; bi-layer RTe-sheets andtwo square Te-sheets are stacked along
the b-axis (space group Cmcm, weakly
orthorhombic structure) [1]. Fermi surfaces consist of inner and outer square
sheets, large regions of which are nested
by a single incommensurate wave-vector
corresponding to the observed latticemodulation. Because of the characteristic quasi-two-dimensional nature of the Te
sheet, the charge-density-wave (CDW) is
formed with an extremely large gap [2].
Despite the extensive studies on the CDW
in recent years, remarkably little is known
about magnetism and low-temperature
properties of CeTe3 . Recently, it has beenreported that CeTe3 exhibits two (magnetic) ordering below TN1 = 3.1 K andTN2 = 1.3 K by the speciﬁc heat and susceptibility measurements, shown in Fig.1(a) [3, 4]. From these measurements, thephase below at TN2 seems to be a spindensity-wave (SDW).
The goal of this work is to determine theorder parameters of the low-temperature
two phases by neutron diffraction technique. A single crystal of m ∼ 0.3 gram
was prepared and put in an aluminum canﬁlled with a He gas. It was cooled down
to 0.7 K using a 3 He cryostat [5]. Neutron
diffraction experiments were performed at
HQR and PONTA in the research reactor
JRR-3.
We have searched magnetic reﬂections of
CeTe3 below TN2 with mesh-scans in a scattering plane of ( H, 0, L). We have foundthe Bragg reﬂection at an incommensurate
reciprocal point Q = (0.18, 0, 1.32) at 0.7
K (below TN2 ). Fig.1 (b) shows temperature dependence of the peak intensities at

Q = (0.18, 0, 1.32), which disappeared at
1.5 K (above TN2 ). The development of
the incommensurate magnetic Bragg peakstrongly supports that the order below TN2
are of itinerant magnetic origin. A series ofexperiments indicate that the magnetic order of CeTe3 develops from the paramagnetic phase to the SDW phase through theintermediate phase with the formation ofheavy quasi-particles.
References[1] Y. Iyeiri et al., Phys. Rev. B 67, 144417(2003); N. Ru et al., Phys. Rev. B 73, 033101(2006).
[2] V. Brouet et al., Phys. Rev. Lett. 93, 126405(2004); H. Komoda et al., Phys. Rev. B 70,
195101 (2004).
[3] G.F. Chen et al., in preparation.
[4] K. Deguchi et al., J. Phys. Conf. Series 150,
042023 (2009).
[5] TAIYO NIPPON SANSO CORPORATION. Tokyo 142-8558, Japan.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 772- 148 -

JAEA-Review 2013-039

1-3-8

Thermal variations of magnetic excitation spectrum in slightly overdoped
Bi2.1 Sr1.9 CaCu2 O8+δM. Matsuura1 , Y. Yoshida2 , H. Eisaki2 , N. Kaneko2 , C.-H. Lee2 and K. Hirota1
1 Department of Earth and Space Science, Faculty of Science, Osaka University, Toyonaka,

560-0043.

2 AIST, 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568

Recently, similar magnetic spectra havebeen reported on several high-Tc families,
La2− x Bax CuO4 (LBCO) [1], La2− x Srx CuO4
(LSCO) [2], and YBa2 Cu3 O6+ x (YBCO) [3],namely, a characteristic hourglass-likemagnetic excitation. There are, however,important differences concerning their
thermal variations of spectra across Tc . In
particular, the magnetic resonance peakin YBCO shows an order-parameter likebehavior in contrast to no clear enhancement of the (π, π)-peak at Tc in the LBCO
and LSCO systems. This discrepancy rises
following question. Which part of magnetic excitation is essential and universal
for high-Tc superconductors? One way
to resolve this issue is to investigate another high-Tc system Bi2.1 Sr1.9 CaCu2 O8+δ(Bi2212).
We explored the magnetic
spectrum in slightly overdoped Bi2212
grown by travelling-solvent-ﬂoating zone
method. Neutron scattering 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 massof aligned crystals is 4.6g (0.71cc), which is
12 times as large as the crystal used in theprevious report[4].
From our previous studies, we know
resonance peak appears at ω = 34 meV
and ( 12 , 12 , −14) in our sample. Upon heating above Tc , the intensity at ( 12 , 12 , −14)
(open circles) keeps on increasing except
a small drop at T = 200 K. This dipstructure at T = 200 K is more clear for thedifference (closed circles) between background (BG: open rectangles) and the intensity at ( 12 , 12 , −14). Here, the backgroundat ( 12 , 12 , −14) was estimated as an aver-age of the intensities at (0.1, 0.1, −14) and(0.9, 0.9, −14). Subtracting temperaturedependent background, the (π, π)-peakkeeps on decreasing with increasing temperature up to 200 K, which roughly agrees
with the onset of pseudogap T ∗ = 150 ∼200 K. This suggests that, in slightly overdoped Bi2212, a large magnetic resonancepeak remains above Tc and disappears
around T ∗ , which could be associated withpre-formed singlet pairs in the pseudogap
phase.
References[1] J. M. Tranquada et al., Nature 429, 534(2004).
[2] N. B. Christensen et al., Phys. Rev. Lett. 93(2004) 147002.
[3] S. M. Hayden et al., Nature 429 (2004) 531.
[4] H. F. Fong et al., Nature (London) 398, 588(1999).

Fig. 1. The temperature dependence of the scattering intensity at ω = 34 meV measured at ( 12 , 12 , −14),
background, and the difference between them.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 777- 149 -

JAEA-Review 2013-039

1-3-9

Inelastic neutron scattering experiment on deuterated halogen-bridged nickel
complex
S. Itoh and T. Yokoo
High Energy Accelerator Research Organization, Tsukuba, 305-0801
I(Q=0.8,E) was deduced, and the differenceof S(E,T=10K) - S(E,T=100K) is plotted inFig. 1(b). The spectrum in Fig. 1(b) should
be magnetic signals at the magnetic zone
center if magnetic response is detected.

intensity (counts/1Mmon)[1] K. Toriumi et al., J. Am. Chem. Soc. 111(1989)2341.
[2] H. Okamoto et al., PRB 54 (1996) 8438.
[3] S. Takaishi et al., J. Am. Chem. Soc. 126(2004) 1614.

2000

E = 3 meVT = 100 K
T = 10 K

(a)

1500

1000

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

Q (1/A)intensity (counts/1Mmon)

The halogen-bridged nickel complex,[Ni(chxn)2Br]Br2(chxn=1R,2Rcyclohexandiamine), has a 1D structure,-Br-Ni(III)-Br-Ni(III)-Br-, along the b-axis[1-2]. This spin structure implies the formation of antiferromagnetically coupled
S=1/2 Heisenberg chains of Ni(III). Recently, this system has been suggested to be
the second d-electron spin-Peiers systemfollowing CuGeO3, and the ﬁrst example
of organic d-electron spin-Peiers system(TTF-CuBDT is a p-electron system). In
fact, a clear splitting of the spectrum below
40 K has been observed in the Br-81 NQR
study [3].
We have initiated inelastic neutron scattering experiments in [Ni(chxn)2Br]Br2, inorder to detect magnetic excitations. In theearly stage of our investigations, we grew
single crystals and tried inelastic neutron
scattering experiments. However, since thesample was not deuterated, local modes
originating from hydrogen were too strong
to detect magnetic excitations.
Very recently, we have successfully synthesized 95%-deuterated polycrystals of[Ni(chxn)2Br]Br2. We measured inelastic
neutron scattering spectra from the 95%deuterated polycrystalline sample on the
triple axis spectrometer PONTA (5G) at
JRR3M in JAEA (Tokai), with Ef = 14.7 meV,by using the collimation, open-80 -80 open, at 10 K and 100 K (below and above
the transition temperature). Although weused 95%-deuterated crystals, the background noise was still high as shown in
Fig. 1(a) (1Mmon roughly corresponds to
5 minutes). In order to reduce the background noise, fully-deuterated crystals are
required. The antiferromagnetic zone center is located at Q = 0.6 A-1. Assuming
the signals at Q = 0.8 A-1 to be the background, the spectrum of S(E) = I(Q=0.6,E) -1000
SZC(E) = [I(Q=0.6) - I(Q=0.8)]10K- [I(Q=0.6) - I(Q=0.8)]100K

(b)
500

0

-500
0

1

2

3

4

5

6

7

E (meV)

Fig. 1. Fig. 1 Inelastic neutron scattering spectra from deterated [Ni(chxn)2Br]Br2 measured on
PONTA with Ef =14.7 meV.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 804- 150 -

JAEA-Review 2013-039

1-3-10Electric Control of Helimagnetic Chirality in CoCr2O4
Y. Kousaka1, M. Nishi2, K. Tomiyasu3, M. Matsuura4, K. Hirota4 T. Yokobori1 and J.
Akimitsu1
1Department of Physics and Mathematics, Aoyama-Gakuin Univ., 5-10-1 Fuchinobe,
Sagamihara 229-8558; 2Institute for Solid State Physics, The Univ. of Tokyo, 106-1 Shirakata,
Tokai 319-1106; 3Department of Physics, Tohoku Univ., Aoba, Sendai 980-8578; 4 Departmentof Earth and Space Science, Graduate School of Science, Osaka Univ., 1-1 Machikaneyama,
Toyonaka 560-0043, Osaka
Ferroelectricity driven by magnetic orderis paid a large attention in the recent studyof multiferroics. A cubic spinel CoCr2O4,
in which magnetic Co2+ ions occupy the
A site and Cr3+ ions occupy the B site,
shows ferrimagnetic ordering below TC =93 K and conical-spiral magnetic ordering
below TS = 26 K. [1] As the spiral magnetic
ordering induces electric polarization,[2,3] the right-handed or left-handed spiralmagnetic structure can be controlled by theelectric polarization.[4] To detect the chiralhelimagnetic structure, polarized neutron
diffraction is powerful method by comparing magnetic satellite intensity of up-spinand down-spin incident neutron beams.
To detect the helimagnetic chirality, we
performed polarized neutron diffraction
experiments on a triple-axis spectrometer
5G (PONTA), JRR-3M, Tokai, Japan. Theenergy of incident neutron beam was 13.7
meV. To make single chiral helimagnetic
domains, we cooled the sample with applying a magnetic ﬁeld of 0.5 T along <0, 0, 1>
and electric ﬁeld of 0 to 0.9 kV/mm along<-1, 1, 0>. After cooling, the magnetic andelectric ﬁeld was turned off and the sample
was set on a goniometer. The data was collected at 10 K. By observing nuclear Bragg
reﬂection of (2, 2, 0), the neutron polarization of incident beam was determined
to be 95.4 %. As shown in Fig. 1, we observed magnetic satellite peak at (2-q, 2-q,0), where the magnetic propagation vector
kmag was (q, q, 0) (q = 0.616). To investigate the helimagnetic chirality, intensity
comparison at (± q, ± q, 2) is necessary. As
the peaktop intensity of (± q, ± q, 2) was
too weak (0.1 cps), we estimated the inten-

sity by subtracting the background intensity from the peaktop intensity. In any electric ﬁeld amplitude, the obtained neutron
polarization in (q, q, 2) was nearly zero,
which indicates the right- and left-handed
magnetic screw domains coexist in equal
ratio. The magnetic domains might be destroyed in the process of turning off themagnetic ﬁeld. Therefore, the additionalpolarized neutron diffraction experiments
under an applied magnetic ﬁeld are now inprogress.
[1] K. Tomiyasu et al.: Phys. Rev. B 70 (2004)
214434.
[2] Y. Yamasaki et al.: Phys. Rev. Lett. 96(2006) 207204.
[3] Y. J. Choi et al.: Phys. Rev. Lett. 102(2009) 067601.
[4] H. Katsura et al.: Phys. Rev. Lett. 95(2005) 057205.

Fig. 1. Omega scan proﬁle in (2-q, 2-q, 0)

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 815- 151 -

JAEA-Review 2013-039

1-3-11

Mechanism of Spontaneous Electric Polarization Flop in TbMnO3
H. Sagayama (A), N. Abe (B), T. Arima (A), K. Iwasa (B)(A)IMRAM, Tohoku univ., (B) Dept. Phys., Tohoku univ
Orthorhombic perovskite TbMnO3 is oneof the typical multiferroic systems. Spontaneous electric polarization (P) along the caxis appears below TC (˜27K) [1]. It originates from the spiral conﬁguration of Mn3+
spins rotating in the bc-plane with propagating vector (0 q 1) (q˜0.27) through aninverse effect of the DM interaction [2,3].
Interestingly, the P//c is turned to thea-axis direction by applying a magnetic
ﬁeld along the a- or b-axis. Magnetic structure analysis and a spin-polarized neutron
diffraction study of 160Gd0.7Tb0.3MnO3strongly suggest that P//a also originatesfrom helical spin structure rotating in theab-plane [4]. It has been pointed out that
anisotropic magnetic moments of Tb3+
play an important role for the complicatedelectric polarization ﬂop [5].
To clarify mechanism of the electric
polarization ﬂop, we have performed
diffractiona spin-polarized-neutron
measurement using the TOPAN installedat
JRR-3.
Heusler(111)-Heusler(111)
monochromator-analyser
conﬁguration
was used. The incident neutron energy
Ei was 80 meV. Collimators were set as
open-80-100-open. A single crystal sample
was mounted in a superconducting magnet with the a- and c-axis in the scattering
plane. The magnetic ﬁeld was appliedalong the b-axis up to 5.5 T.
We observed magnetic ﬁeld dependencesof spin-ﬂip and non-spin-ﬂip scattering at(0, q, 7) and (4, q, 1) at 8 K. These results
indicate the basal plane change of spin helix from the bc- to ab- plane. In addition,
we observed increasing of (1 0 6) reﬂection corresponding to the C-type antiferromagnetic structure with increasing magnetic ﬁeld. It might be caused by the local
anisotropy of Tb magnetic moments lying
in the ab plane. Based on the experimental
results, we considered coupling between

Mn3+ spins and anisotropic Tb3+ magnetic
moments. We calculated magnetic ﬁeld dependence of the energy gain of the coupling and succeeded in reproducing theelectromagnetic diagram of TbMnO3 [5].
Reference[1] T. Kimura et al., Nature (London) 426,
55 (2003).
[2] M. Kenzelmann et al., Phys. Rev. Lett.
95, 087206 (2005).
[3] Y. Yamasaki et al., Phys. Rev. Lett. 98,
147204 (2007).
[4] Y. Yamasaki et al., Phys. Rev. Lett. 101,
097204 (2008).
[5] N. Abe et al., Phys. Rev. Lett. 99, 227206(2007).

Fig. 1. Magnetic ﬁeld dependences of integrated intensities of (1 0 6) and (3 0 0) refrection. The inset
shows reﬂection proﬁles of spin frop and non-spin
ﬂop scattering at (1 0 6).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 829- 152 -

JAEA-Review 2013-039

1-3-12

Thermoelectric properties and crystal structures in layered Co oxides
H. Nakatsugawa and K. Nagasawa
Yokohama National University 79-5 Tokiwadai Hodogaya-ku Yokohama 240-8501 Japan
Polycrystalline samples were prepared bya conventional solid-state reaction method.
Appropriate amount of starting from a
mixture of CaCO3 (99.9%) and Co3O4(99.9%) powders were mixed with an agate
mortar and pressed into pellets. The pellets were calcined in air at 920 ℃ for
12h and sintered at 920 ℃ for 24h under pure ﬂowing oxygen gas. The samples were furnace cooled to room temperature, ground and pelletized again. This process was repeated three times in order toobtain well-crystallized single-phase sample. In addition, one of the obtained wellcrystallized single-phase samples were annealed in pure ﬂowing Ar gas at 740 ℃ for
48h and then quenched in distilled water tocontrol oxygen nonstoichiometry δ. In thiswork, we prepare two samples: ”Sample
A” and ”Sample B”. The former is the obtained well-crystallized single-phase sample, and the latter is the annealed sample tocontrol oxygen nonstoichiometry δ in reduction atmosphere.
Neutron powder diffraction (ND) data
were collected at room temperature usinga Kinken powder diffractometer for thehigh-efﬁciency and high-resolution measurements (HERMES) of Institute for Materials Research (IMR), Tohoku University,
installed at a JRR-3M reactor in Japan
Atomic Energy Research Institute (JAERI).
The ND data were collected on thoroughly ground powders in a multiscanning mode in the 2 θ range from 3.0
to 153.9 °with a step width of 0.1 °.The
incident neutron beam was monochromatized to a wavelength of 1.8205 Å.The
XRD and ND data were simultaneously
analyzed using a Rietveld reﬁnement program PREMOS 91 designed for modulated
structure analyses. We adopt a superspacegroup of C2/m(1p0)s0 because the CdI2type [CoO2] subsystem has a C2/m sym-

metry, whereas the RS-type BL subsystem
has a C21/m symmetry. The crystal structures and interatomic distance plots wereobtained using the PRJMS and MODPLT
routines, respectively; both are included in
the PREMOS 91 package.
Figure 1(a) shows the observed, calculated
and difference intensities of the HERMES
data for Sample A. Short vertical lines below the patterns indicate the peak positionsof the main (upper) and satellite (lower) reﬂections of the two subsystems. The ﬁnal
Rwp factor is 5.37 % and the lattice parameters are reﬁned to a = 4.83353(4) Å, bCoO2= 2.82380(7) Å, c = 10.8455(3) Å and β= 98.141(5) °for the [CoO2] subsystem andbRS = 4.55757(8) Å for the RS-type BL subsystem. The resulting p = bCoO2/bRS =0.61958(5) 〜0.62 corresponds to the structural formula [Ca2CoO3.08]0.62CoO2.
The crystal structure of Sample B was also
analyzed in a similar manner. Figure 1(b)shows the observed, calculated and difference intensities of the HERMES data for
Sample B. Short vertical lines below thepatterns indicate the peak positions of themain (upper) and satellite (lower) reﬂections of the two subsystems. The ﬁnal Rwp
factor is 4.69 % and the lattice parameters
are reﬁned to a = 4.83804(6) Å, bCoO2 =2.82533(1) Å, c = 10.86027(2) Å and β =98.135(8) °for the [CoO2] subsystem andbRS = 4.55128(9) Å for the RS-type BL subsystem. The resulting p = bCoO2/bRS =0.62077(6) 〜0.62 corresponds to the structural formula [Ca2CoO3.08 −δ]0.62CoO2.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 833- 153 -

JAEA-Review 2013-039

Fig. 1. Fig.1 Observed, calculated and difference intensities of powder ND data for (a) Sample A and(b) Sample, respectively.The inset is the ﬁnal crystal
structure.

1-3-12- 154 -

JAEA-Review 2013-039

1-3-13

Thermoelectric properties and crystal structures in layered Co oxides
H. Nakatsugawa and K. Nagasawa
Yokohama National University 79-5 Tokiwadai Hodogaya-ku Yokohama 240-8501 Japan
Polycrystalline samples were prepared bya conventional solid-state reaction method.
Appropriate amount of starting from a
mixture of CaCO3 (99.9%) and Co3O4(99.9%) powders were mixed with an agate
mortar and pressed into pellets. The pellets were calcined in air at 920 ℃ for
12h and sintered at 920 ℃ for 24h under pure ﬂowing oxygen gas. The samples were furnace cooled to room temperature, ground and pelletized again. This process was repeated three times in order toobtain well-crystallized single-phase sample. In addition, one of the obtained wellcrystallized single-phase samples were annealed in pure ﬂowing Ar gas at 740 ℃ for
48h and then quenched in distilled water tocontrol oxygen nonstoichiometry δ. In thiswork, we prepare two samples: ”Sample
A” and ”Sample B”. The former is the obtained well-crystallized single-phase sample, and the latter is the annealed sample tocontrol oxygen nonstoichiometry δ in reduction atmosphere.
Neutron powder diffraction (ND) data
were collected at room temperature usinga Kinken powder diffractometer for thehigh-efﬁciency and high-resolution measurements (HERMES) of Institute for Materials Research (IMR), Tohoku University,
installed at a JRR-3M reactor in Japan
Atomic Energy Research Institute (JAERI).
The ND data were collected on thoroughly ground powders in a multiscanning mode in the 2 θ range from 3.0
to 153.9 °with a step width of 0.1 °.The
incident neutron beam was monochromatized to a wavelength of 1.8205 Å.The
XRD and ND data were simultaneously
analyzed using a Rietveld reﬁnement program PREMOS 91designed for modulated
structure analyses. We adopt a superspacegroup of C2/m(1p0)s0 because the CdI2type [CoO2] subsystem has a C2/m sym-

metry, whereas the RS-type BL subsystem
has a C21/m symmetry. The crystal structures and interatomic distance plots wereobtained using the PRJMS and MODPLT
routines, respectively; both are included in
the PREMOS 91 package.
Figure 1(a) shows the observed, calculated
and difference intensities of the HERMES
data for Sample A. Short vertical lines below the patterns indicate the peak positionsof the main (upper) and satellite (lower) reﬂections of the two subsystems. The ﬁnal
Rwp factor is 5.37 %. The crystal structureof Sample B was also analyzed in a similarmanner. Figure 1(b) shows the observed,
calculated and difference intensities of the
HERMES data for Sample B. Short verticallines below the patterns indicate the peak
positions of the main (upper) and satellite(lower) reﬂections of the two subsystems.

Fig. 1. Observed, calculated and difference intensities of powder ND data for (a) Sample A and (b)Sample B, respectively. The inset is the ﬁnal crystal
structure.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 835- 155 -

JAEA-Review 2013-039

1-3-14

Nonmagnetic impurity eﬀect in ferroelectric phase of CuFeO2
T. Nakajima1 , S. Mitsuda1 , M. Yamano1 , H. Yamazaki1 , M. Matsuura2 , K. Hirota2
1 Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601
2 Department of Earth and Space Sci., Osaka University, Toyonaka 560-0043

In the past several years, a magnetic oxide CuFeO2 (CFO) has been intensively
investigated as a new class of magnetoelectric (ME) multiferroics, whose ferroelectricity is originated from a properscrew type magnetic ordering. The recent
experimental studies have revealed thatthe ferroelectric helimagnetic phase, which
originally shows up as a magnetic-ﬁeldinduced phase in pure CFO, also shows
up as a ground state in slightly diluted
CuFe1− x Alx O2 (CFAO) and CuFe1− x Gax O2(CFGO). Although the origin of the ferroelectricity must be common to CFO, CFAO
and CFGO, the reported values of the observed macroscopic electric polarization, P,
are rather different from each other. In
particular, the previously reported value of
P in CFAO (∼ 50μC/m2 ) is remarkably
smaller than the values in CFO and CFGO
(200 ∼ 400μC/m2 ).
In the present study, we have thus
performed polarized neutron diffraction
and in-situ pyroelectric measurements on
CFAO, in order to answer the question:”What determines the magnitude of P in
CFO, CFAO and CFGO systems?”. The polarized neutron diffraction measurements
on CFAO(x = 0.015) were carried out at the
triple-axis neutron spectrometer PONTA
installed by University of Tokyo at JRR-3
in the Japan Atomic Energy Agency(JAEA).
Incident polarized neutron beam with energy 34.06 meV was obtained by a Heusller(111) monochromator. The ﬂipping ratioof the polarized neutron beam was ∼ 14.
The experimental settings and procedures
including pyroelectric measurement were
the same as those in the previous polarized
neutron diffraction measurement on CFAO
(x = 0.02).[3]Since our previous work have revealed
a one-to-one correspondence between thespin helicity and the polarity of the induced
ferroelectric polarization, in the present
work, we have deduced asymmetry in
the fractions of the left-handed and righthanded helical magnetic ordering from theresults of the polarized neutron measurements. We refer to this asymmetry of thespin helicity as D.
Figures 1(a-1) and 1(a-2) show the measured values of D and P as functions of
E p . We found that P and D in CFAO
were rather insensitive to E p . However,
we also found that CFAO can achieve P of
∼ 250μC/m2 , which is comparable to thevalues of P in CFO and CFGO, as shown in
the inset of Fig. 1(b). This implies that themagnitude of the local electric polarizationin CFO system does not reduced by the Alsubstitution, but the sensitivity of P to E p is
reduced.
References[1] T. Kimura et al.: PRB 73 220401(2006).
[2] T. Nakajima et al.: JPSJ 76 (2007)043709.
[3] T. Nakajima et al. PRB 77 052401 (2007).

Fig. 1. [(a)-(b)] E p dependences of (a)P and (b)D in
CFAO (x = 0.015) at T = 2.0K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 849- 156 -

JAEA-Review 2013-039

1-3-15Magnetic Phase Diagram in Ba2 Mg2 Fe12 O22
H. Sagayama(A), K. Taniguchi(A), T. Arima(A), Y. Nishikawa(B), S. Yano(B), J.
Akimitsu(B), M. Matsuura(C), K. Hirota(C)(A)IMRAM, Tohoku Univ., (B)Dept. Phys., Aoyama-Gakuin University, (C)Dept. Earth andSpace Science, Osaka Univ.
It has been recently found that a Ytype hexaferrite Ba2 Mg2 Fe12 O22 (BMFO)
exhibits a nonlinear magnetoelectric effect[1,2]. It is proposed that the conical magnetic structure at low temperatures is modiﬁed by the application of a weak magnetic
ﬁeld perpendicular to the cone axis of thec axis, which produces the electric polarization. However, the magnetic phase diagram of BMFO has not been clariﬁed yet.
We performed a neutron diffraction measurement to reveal the magnetic phase diagram with the H  b∗ conﬁguration.
Single crystals of BFMO were grownfrom Na2 O-Fe2 O3 ﬂux. Neutron diffraction
measurement was performed with a tripleaxis neutron spectrometer PONTA at JRR3. A single crystal was set in a 4 He refrigerator. A magnetic ﬁeld was applied parallelto the b-axis using a 1T electromagnet. The
diffraction proﬁle along (1 0 L) was measured for various temperatures and magnetic ﬁelds.
As cooling down the sample down to
10 K in zero magnetic ﬁeld, clear magnetic satellite peaks are observed at L=-3.4
and -1.6, indicating a incommensurate conical phase. Considering the M-H curve,
the cone axis is possibly parallel to thec-axis. As increasing the magnetic ﬁeld
along the b-axis to 0.2 T, the peak positionof the magnetic satellites suddenly moves
to L=-4.5. The compound clearly undergoes incommensurate-commensurate magnetic phase transition. A magnetic structure analysis with using FONDER suggeststhat the magnetic moments form a spiralaround the b axis and propagate along thec axis with a period of two unit layers.
The magnetic structure does not change
at least up to 0.5 T. With decreasing themagnetic ﬁeld down to 0 T, the magnetic

structure does not show the incommenratealignment but changes to another commensurate phase. The period of the magneticalignment is six unit layers.
At higher temperatures, we also ﬁnd thefour-fold magnetic phase for an intermediate region between the low-ﬁeld six-foldphase and high-ﬁeld two-fold phase. We
summarize the magnetic phase diagram in
Fig. 1.
References[1] K. Taniguchi et al., Appl. Phys. Express 1, 031301 (2008).
[2] S. Ishiwata et al., Science 319, 1643
(2008).

Fig. 1. Magnetic phase diagram of a Y-type hexaferrite Ba2 Mg2 Fe12 O22 for magnetic ﬁelds along theb-axis.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 851- 157 -

JAEA-Review 2013-039

1-3-16

Magnetic Property of Prx Fe4 Sb12
K. Iwasa1 , T. Orihara1 , Y. Murkami1 ,K. Kuwahara2 , H. Sugawara3
Tohoku Univ.1 , Ibaraki Univ.2 , The Univ. of Tokushima3
we succeeded in observing the increase offundamental reﬂection intensities with decreasing temperature thorough the transition temperature. This results is consistent
with the previous study, and the magnetic
ordering pattern is composed of ferromagnetic component. However, because of thesmall single crystalline sample, we have
not yet achieved to the conclusion of magnetic structure. We will carry out a subsequent measurement with a larger volume
sample.
The less dependence of the 4 f crystal
ﬁeld levels and the apparent dependenceof the magnetic ordering on the Pr ion concentration may indicate that the magnetic
ordering is predominated by Fe magnetic
moments as discussed previously.
60
Q = 3.0 (2π/a)
3.3 K
Pr
La

Counts / 1200 MN (2 min)

50

200

40

150

30
100
20

Counts / 120 MN (elastic region)

Rare-earth ﬁlled skutterudite compounds have been studied for various
phase transitions of 4 f electron states.
Prx Fe4 Sb12 has been considered to exhibit
magnetic ordering at around 4 K, that iscomposed by not only Pr 4 f but also Fe
3d electrons (N. P. Butch et al.: Phys. Rev.
B 71 (2005) 214417), since the magnitudeof effective magnetic moment estimatedfrom the high temperature magnetic susceptibility is larger than that of Pr3+ freeion. The ordered structure of the twokinds of magnetic moments depending on
the Pr ﬁlling has been unsolved yet. It isnotable that the magnetic phse transition
is reported to disappear in case of fulloccupation of the Pr-ion sites (x = 1). The
effect of Pr ﬁlling to the magnetic ordering
has also not been explained.
We performed neutron scattering experiment using the triple-axis spectrometer
TOPAN (6G) in order to reveal Pr-ion crystal ﬁeld levels by using powdered simple
and the four-circle diffractometer FONDER(T2-2) to investigate the magnetic orderedstructure by using a single crystalline sample. These samples were synthesized by theso-called Sb-self ﬂux method, and the Pr
concentration x is expected to be less thanunity (x = 0.7 − 0.9), as was reported
in the previous reports. Figure shows inelastic spectra observed at TOPAN. We succeeded in observing two magnetic excitation peaks at 2.4 and 11 meV. The peak positions are almost equivalent with those of
the x < 1 sample reported by E. Bauer etal. (J. Magn. Magn. Mater. 310 (2007)286) but also for the x 1 one synthesized
by K. Tanaka et al. using the high-pressure
method (J. Phys. Soc. Jpn. 76 (2007)
103704). Therefore, one can expect that thenature of 4 f electrons localized at Pr ionsdoes not strongly depend on the Pr ion concentration. In the Experiment at FONDER,

50
10

0
-2

0

2

4

6

8

10

12

14

0
16

Energy [meV]Fig. 1. Magnetic excitation spectra of Prx Fe4 Sb12
and Lax Fe4 Sb12 at 3.3 K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 859- 158 -

JAEA-Review 2013-039

1-3-17

Crystal-ﬁeld excitation and multipolar ordering in Pr(Ru1−x Rhx )4 P12
K. Iwasa1 , K. Saito1 , L. Hao2 , Y. Murakami1
Tohoku Univ.1 , China Institute of Atomic Energy2
appearing in the Rh doped systems indicate appearance of Pr ions without contribution to the ordering. In order to identify the level schemes produced by the Rh
doping, we carried out the inelastic measurements under magnetic ﬁeld for the x= 0.05 system. Figure depicts the magnetic ﬁeld dependence of the excitation at
2.4 meV measured at 1.6 K. The broadening and asymmetric shape of the peak under ﬁnite magnetic ﬁeld indicate that thepeak corresponds to excitation from singlet
ground state to triplet state. On the phasetransition to the antiferro-type hexadecapolar ordering in the pure system, the crystal
ﬁeld level scheme at one of the Pr ion sites
switches from a singlet to a triplet state.
Thus, the Rh doping is thought to force thePr 4 f electron state to remain at the singlet
state, resulting into the suppression of thetransition.
250
Pr(Ru0.95Rh0.05)4P12Counts / 6000 MN (1090 sec)

Spontaneous ordering of higher-rank
multipoles of 4 f electrons has been detected in various rare-earth based materials. PrRu4 P12 is one of typical systems,
exhibiting the antiferro-type hexadecapolar (rank-4 multipolar) ordering below themetal-nonmetal transition at 63 K (T. Takimoto: J. Phys. Soc. Jpn. 75 (2006) 034714).
The phase transition is a new type of charge
density wave formation originating fromthe coupling of the Fermi surface nesting
property to the modulated 4 f multipolar
arrangement. This coupling is due to p- f
hybridization between 4 f and conduction
electrons. It should be notable that the ordering is characterized by the crystal ﬁeld
excitations exhibiting the strong temperature dependence in accordance with theevolution of the multipolar order parameter (K. Iwasa et al.: Phys. Rev. B 72 (2005)
024414). The substitution of Rh to Ru gives
rise to rapid suppress of metal-nonmetaltransition; the electrical resistivity at low
temperature in the Rh 10% system becomes
the same magnitude at around 60 K (C.
Sekine et al.: Physica B 378-380 (2006) 211).
Thus, a study of the doping effect leads tounderstand the ordered 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 have performed experiments using
the triple-axis spectrometers HER (C1-1)
and TOPAN (6G) for polycrystalline sample of Pr(Ru1− x Rhx )4 P12 . These previous
studies revealed that the Rh doping systems (x = 0, 0.03, 0.05, 0.10 and 0.15)
shows the crystal ﬁeld excitations at 2.4
and 13 meV, whose peak positions do notshow any temperature dependence, in addition to the strongly temperature dependent ones. The most recent measurement
for x = 0.01 performed at HER also shows
the same excitation spectrum. The peaks

200

150

100

T = 1.6 K
0T
5T
2.5 T

50

0

0

1

2

3

4

Energy [meV]Fig. 1. Magnetic ﬁeld dependence of crystal-ﬁeld excitations of Pr(Ru0.95 Rh0.05 )4 P12 at 1.6 K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 860- 159 -

JAEA-Review 2013-039

1-3-18

Electric Field Control of Magnetic Correlation in Multiferric Cu(Fe,Al)O2
K. Takahashi, Y. Kaneko, T. Ito, T. Nakajima, and S. Mitsuda
Department of Physics, Faculty of Science, Tokyo University of Science, Tokyo 162-8601
Recently, a magneto-electric multiferroic
CuFeO2 , in which the ferroelectric phaseshows up as a magnetic-ﬁeld- or impurityinduced phase, has been extensively investigated. The recent experimental works
have revealed that the magnetic structurein the ferroelectric phase is a ‘proper-screwtype’ structure[1], whose spin-helicity corresponds to the polarity of the local ferroelectric polarization emerging along thehelical axis.[2] In the previous neutron
diffraction measurement on CuFe1− x Alx O2
at FONDER(T2-2),[3] we have discoveredthat magnetic diffraction proﬁles in the ferroelectric phase were sharpened by applying electric ﬁeld parallel to the helical axis.
This implies that the magnetic correlation
length in the ferroelectric phase can be controlled by an applied electric ﬁeld.
In order to investigate the electric ﬁeld
dependence of the magnetic correlation
length in detail, in the present experiment, we have performed neutron diffraction measurements on CuFe1− x Alx O2 (x =0.02) under applied electric ﬁelds parallel and perpendicular to the helical axis,
using the triple-axis neutron spectrometers HQR(T1-1) and HER(C1-1) installed at
JRR-3. As shown in Figs. 1(a) and 1(b),we found that a poling electric ﬁeld applied parallel to the helical axis sharpens
the diffraction proﬁle of (q, q, 3/2) magnetic reﬂection in the ferroelectric phase,but that applied perpendicular to the helical axis does not. Figure 1(c) shows that thevariance of the diffraction proﬁle, whichis relevant to the inverse magnetic correlation length, decreases, with increasing poling electric ﬁeld. This suggests that the average size of the magnetic domains is enlarged by the poling electric ﬁeld, owing
to the one-to-one correspondence between
the magnetic and ferroelectric domains, because the poling electric ﬁeld should en-larges the ferroelectric domains in which
the local electric polarization is parallel toit. Note that this electric ﬁeld dependenceof the magnetic correlation length might
not be observed not in the typical multiferroics such as TbMnO3 , but is clearly observed in CuFe1− x Alx O2 . This is because
the magnetic correlation in the ferroelectric phase of CuFe1− x Alx O2 (x = 0.02) isoriginally disturbed by site-random Al3+ substitutions, and therefore the change inthe magnetic correlation length was easily
detected by neutron diffraction measurements. For further research, we will investigate the helicity-dependent magnetic correlation by polarized neutron diffraction
measurements.
References[1] T. Nakajima et al.: JPSJ 76 043709 (2007).
[2] T. Nakajima et al.: PRB 77 052401 (2008).
[3] T. Nakajima et al.: ISSP-NSL report #328
(2007).

Fig. 1. (a)(b)Diffraction proﬁles in the ferroelectricphase. Green bar stand for resolution limit. (c)Eﬁeld dependence of the variance of diffraction proﬁles in the ferroelectric phase and the polarization.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 877- 160 -

JAEA-Review 2013-039

1-3-19Rattling vibration of cage compounds
C. H. Lee(A), H. Yoshizawa(B), K. Kihou(A), T. Onimaru(C), K. Suekuni(C), T.
Takabatake(C)(A) AIST, (B) ISSP, (C) Hiroshima Univ.
with the acoustic phonon mode, though thegap energy is relatively small comparing
with that of Ba8Ga16Ge30. Analysis basedon a Born-von Karman force model has
clariﬁed that the Sr atoms are bound very
weakly to surrounding atoms, with a force
constant of 0.007 ˜ 0.009 mdyn/A. The results suggest that hybridization between
the guest atoms and host lattice vibration
is weak in Sr8Ga16Ge30 compounds.
[1] C. H. Lee et al., J. Phys. Soc. Jpn. 77(2008) 260, Suppl. A.
[2] C. H. Lee et al., J. Phys.: Conf. Ser. 92(2007) 12169.

  

A large vibration of an atom in an oversized atomic cage, so called rattling, has attracted great interest since it can be the origin of exotic physical properties. For example, rattling can be responsible for the extremely low thermal conductivity in cagecompounds. Electronic properties could
be also affected by rattling via electronphonon coupling. To clarify the effect ofrattling motion on these exotic physicalproperties, it is very important to understand the nature of rattling.
Type-I clathrate X8Ga16Ge30 (X=Ba, Sr
or Eu) is one of compounds that has large
Ga and Ge atomic cages ﬁlled with X guest
atoms. According to crystal structure analysis, the positions of Sr and Eu atoms
split into four sites. Phonon dynamics ofcage compounds with off-centered guest
atoms are a controversial issue. Therefoire, we studied the phonon dynamics of
Sr8Ga16Ge30 by inelastic neutron scattering [1,2].
Neutron scattering measurements werecarried out using a triple-axis spectrometer, TOPAN, at the JRR-3 reactor of JAEA at
Tokai. The ﬁnal neutron energy was ﬁxed
at Ef=14.8 meV using a pyrolytic graphite(PG) monochromator and analyzer. The sequences of horizontal collimators were 40’30’-S-30’-30’ where S denotes the sample
position. A single crystal of Sr8Ga16Ge30
was grown by a self-ﬂux method using excess Ga. The volume of the single crystal
used for the measurements was about 2 cc.
All measurements were conducted at room
temperature.
Figure 1 shows the phonon dispersionof Sr8Ga16Ge30 with propagation vector of[100]. The optical phonon mode observed
at E = 4 meV corresponds to a guest mode,in which Sr atoms vibrate largely. The
guest mode shows anti-crossing behavior














Fig. 1. Phonon dispersion curves of transverse
acoustic and optical phonon modes with propagation vector [100] in Sr8Ga16Ge30.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 882- 161 -

JAEA-Review 2013-039

1-3-20Spin ﬂuctuations of single-layer in Bi2+xSr2-xCuO6+d superconductor
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, Japantuations below 11 meV in the x=0.2 sample (hole concentration is ∼0.17). Interestingly, the magnetic signals were observed
at (0.5±δ, 0.5)/(0.5, 0.5±δ) with δ∼0.12(r.l.u.) in the tetragonal notation, whichis consistent with those reported for LSCO
system with comparable carrier concentration [3]. This observation of incommensurate structure in the single-layer Bi2201
provides provides important opportunity
to explore the generic feature of spin excitation spectra in high-Tc cuprates.
References[1] J. M. Tranquada et al.: Nature 375 (2004)
531.
[2] S. M. Hayden et al.: Nature 375 (2004) 534.
[3] K. Yamada et al.: Phys. Rev. B 57 1998) 6165.

Bi2.2Sr1.8CuO6+δ, T=70K
600(0.5 k 0)500
400Counts/22min

Inelastic neutron-scattering measurement is a powerful technique for the
study of spin dynamics and lattice vibrations (phonon) in condensed matterssuch as high-Tc superconductors. Systematic neutron-scattering experiments on
the high-Tc superconducting systems ofLa2− x Srx CuO4 (LSCO) and YBa2 Cu3 O6+δ(YBCO) revealed an existence of similardispersion in the spin excitation spectrum [1, 2]. Therefore, the spin correlationis considered to closely connect with thesuperconductivity. On the other hand, aninteraction of the phonon and the electron
seems to be also important in the high-Tc
superconductor because anomalous softening in the bond-stretching phonons wereobserved in the superconducting phase ofboth LSCO and YBCO systems. Thus, theorigin of pairing force for the emergenceof high-Tc superconductivity, namely spin
ﬂuctuations, phonon and others, is still
discussed. However, since the high-Tc
superconducting systems studied byneutron-scattering experiments are quite
limited, other reference systems are highly
required for the clariﬁcation of universal
nature in spin excitations and phonons.
Motivated by the above reason, we havestarted the study on Bi2+ x Sr2− x CuO6+δ
(Bi2201) system.
The crystal growth of Bi2201 superconductor is known to be much difﬁcult thanthat of LSCO and there is no report on thespin dynamic and phonon investigated byneutron-scattering measurement. We have,
however, found adequate growth condition of sizable single crystal, and succeededin observing inelastic magnetic signals in
Bi2201 system for the ﬁrst time.
Figure 1. shows the low-energy spin ﬂuc-

300

500
400

ω=4meV(h 0.5 0)

ω=11meV

300
200
0.1

0.3

0.5

0.7

0.9

q (r.l.u.)
Fig. 1.
Inelastic neutron scattering spectra of
Bi2.2 Sr1.8 CuO6+δ with constant energy of 4 meV and
11meV measured at 70K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 891- 162 -

JAEA-Review 2013-039

1-3-21

Dual structure in spin excitations of La2-xSrxCuO4 studied through impurity eﬀect
M. Fujita1 , M. Enoki2 , S. Iikubo3 , and K. Yamada3
1 Institute for Materials Research, Tohoku University, Katahira, Sendai 980-8577, Japanpressed. This result suggests that the spectral weight is shifted toward the low energy
side by Fe-doping, and therefore, the low
energy component is signiﬁcantly affectedby Fe-doping. To conclude the existenceof dual nature of spin excitations, study of
Fe-doping effects on the high-energy is required, and the neutron-scattering experiment is now under progress.
References[1] B. Vignolle et al.: Nature Physics 3,(2007)163.
[2] D. Reznik et al.:Phys. Rev. B 78
(2008)132503.
[3] Y. Bang: arXiv:cond-mat/0706.1387.
[4] M. Kofu et al.: Phys. Rev. Lett. 102(2009)047001.
3

χ" (arb. unit)

Antiferromagnetism in the doped
cuprate Mott-insulator has been extensively investigated due to its rich physics
and close relation with the high transition
temperature (high-Tc) supercoductivity.
Recently, Vignolle and co-workers revealed the existence of two energy scales
in the spin excitations of optimally doped
La1.64 Sr0.16 CuO4 exhibiting the sharp andbroad intensity-maximum at 18meV and
45meV, respectively [5].
Furthermore,even in the optimally-doped region of
Y-123 existence of high-energy dispersive
magnon-like modes, which is not reproduced by the Fermi liquid theory wasreported [6], while the low-energy spin
dynamics including resonance feature iswell explained by fermiological way. Suchstructure of spin excitation showing dual
nature suggests the different origins forthe hourglass-shape spectrum separated
by energy. Indeed, phenomenological theory, which treats both itinerant fermionsand local spins have well reproduced theoverall spin susceptibility in Y-123 [7].
Therefore, two spin degrees of freedomof the itinerant spins and local spins
would intrinsically exist in the high-Tc
compounds. To make progress on above
issue, we investigated the spin excitations
in Fe-doped La2− x Srx CuO4 system, inwhich both spin and charge stripe order issigniﬁcantly stabilized by Fe-doping.
In Fig. 1, the local spin susceptibility (χ )is plotted for La1.64 Sr0.16 Cu0.98 Fe0.01 O4 .
With decreasing the energy transfer (ω), χ
below 6 meV decreases toward the minimum intensity at ∼2 meV and turn to increase, showing a gap-like structure. Compared to the Fe-free LSCO with the comparable hole concentration shown by dashedline, the low-energy component below 2
meV is strongly enhanced while the highenergy component above 8 meV is sup-LSCO,
x=0.14

2

1

0

0

5

ω (meV)

10

Fig. 1.
Local spin susceptibility forLa1.94 Sr0.16 Cu0.98 Fe0.02 O4
measured at 14K.
Dashed line represents the result for Fe-free LSCO
with the comparable hole concentration.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 895- 163 -

JAEA-Review 2013-039

1-3-22

Doping evolution of spin correlations in electron-doped Pr1-xLaCexCuO4
M. Fujita1 , J. Kaminaga2 , 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, Japansuggest that the commensurate spin correlations are closely related with the superconductivity in the n-type cuprates.
References[1] K. Yamada et al., Phys. Rev. Lett. 90(2003)137004.
[2] J.A. Skinta et al.: Phys. Rev. Lett 88(2002)207005.
[3] V.A. Khodel et al.: Phys. Rev. B 69
(2004)144501.
Pr1-xLaCexCuO4+δ, T=8K
ω=10-11meV
ω=4meVCount/8min Counts/7min Count/7min Count/11min

(a)

300

x=0.07200

300

x=0.07(h h 0)

200

100

100

0
400

0

x=0.09x=0.09

200

200

0

0

x=0.15x=0.15

200

400

200

100

0
400

0

x=0.18x=0.18

50K

100

200

0
0.40

0.45

0.50

0.55

0.60 0.40

0.45

0.50

0.60

0.55

h (r.l.u.)(b)2.4

2.4

0.8

1.6
0.8

x=0.07

χ (ω) (μB2 /eV /f.u.)

00

x=0.18

1.6
0.8

1.6
0.8

x=0.090x=0.111.6

05

ω (meV)1015

x=0.130.8

x=0.0920
10x=0.180

510

ω (meV)

15 0

2

30

Tc (K)

x=0.11x=0.13x=0.15

0

0
40

0.8

1.6

χ (ω) (μB2 /eV /f.u.)

x=0.151.6

00Count/11min Count/6min Counts/10min Count/10min

Antiferromagnetic (AF) spin ﬂuctuations
are widely believed to play a crucial role
for the appearance of high temperature superconductivity in cuprates. Neutron scattering experiments have revealed the existence of low-energy spin ﬂuctuations in the
superconducting phase of electron-dopedNd2− x CexCuO4 and Pr1− x LaCexCuO4 [1].
On the other hand, an evidence for thetransition or crossover of superconducting paring symmetry from being d-wave
to s-wave in nature upon doping wasreported for the electron-doped (n-type)cuprate [2, 3]. This suggests that in the
n-type superconductors the d-wave superconductivity mediated by spin ﬂuctuations
can change to the conventional s-wave superconductivity mediated by lattice vibrations with increasing doping concentration.
Since the observed spin correlation in theelectron-doped cuprate is limited to the
optimally-doped region, the doping evolution of spin correlation in the superconducting phase is necessary to determine
whether the crossover of paring symmetry occurs or not. We, therefore, investigated the low-energy spin ﬂuctuations inPr1− x LaCex CuO4+δ over a wide concentration range of 0.07≤ x ≤0.18, spanning fromthe antiferromagnetic phase to the heavily
overdoped superconducting (SC) phase.
As seen in Fig. 1(a), the low energy excitations exhibit commensurate peaks centered at the (π, π) position, unlike to the incommensurate one in the hole-doped system. Figure 1(b) shows the imaginary partof the dynamic susceptibility, χ (ω ), as afunction of ω. In the SC phase with x ≥0.11, the relaxation rate of the spin ﬂuctuations corresponding to the peak-energy islinearly proportional to Tc . These results

x=0.074

Γ (meV)

6

8

0Fig. 1. (Upper panels) Constant-ω scans with ω = 4
meV and 10-11 meV. (Lower panels) ω-dependenceof the local spin susceptibility and Tc as a functionof Γ.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 906- 164 -

JAEA-Review 2013-039

1-3-23

Crystal structure of the calcium-ferrite type 1-D chain compounds CaCo2O4
Masaaki ISOBE (A), Yoshitaka MATSUSHITA (B)(A) Superconducting Materials Center, National Institute for Materials Science; (B) Quantum
Beam Center, National Institute for Materials Science
The CaFe2O4 (calcium ferrite)-type structure can be described using a general formula AB2O4 (A= alkali or alkali-earth ion;
B= transition-metal ion), which crystallizes in an orthorhombic structure with lattice constants a˜9 A, b˜3 A, and c˜10 A(space group: Pnma), built of eight-foldcoordinated A atoms and distorted BO6octahedra. The BO6 octahedra form anedge-sharing one-dimensional (1-D) double chain network along the b-axis, inwhich unique quantum behavior characteristic of low-dimensional system may occur due to strong correlation between electrons. Recently, we found a new memberof the calcium-ferrite-type structure family,
CaCo2O4 ± d, by utilizing high-pressure
synthesis technique, and found that thecompound can exhibit comparatively large
thermoelectric power (>150 microV/K),
even though it has ﬁnite density of statesat Fermi level [1]. This large thermoelectric
power may be attributed to residual spin
entropy due to orbital degeneration, or distinctive dispersion of the Co t2g bands
around Fermi level [2]. In this short paper,
we report structural parameters precisely
reﬁned using Rietveld analysis with neutron diffraction data, and evaluate bond valences of the Co ions in order to ﬁnd which
crystallographic site, Co1 or Co2, is prior toanother site for hole doping.
Polycrystalline sample of CaCo2O4 prepared from a solid-state reaction under 7.7
GPa and 1,600 °C was used for the neutron
diffraction experiments. Diffraction data
were collected using the HERMES diffractometer (IMR, Tohoku Univ.) at room temperature in a step size of 0.1 deg. over a2theta range of 3-152.9 deg. using 150 3He
counters set at 1 deg. intervals. Incident
thermal neutron beams were monochromatized to a wavelength of 1.8204 A withthe 331 reﬂection of a bent-crystalline Ge
monochromator. Structural reﬁnement was
performed using the Rietveld analysis program RIETAN-2000 [3]. Initial structure
models and parameters were constructedusing the results of the X-ray Rietveld analysis in ref. 1.
Figure 1 shows a powder neutron
diffraction pattern of CaCo2O4 for the
Rietveld analysis. Some of small extra
reﬂections were purposely excluded
from the observed data to improve thereliability factors. The data elimination
between 77.0 and 77.9 deg. is due to machine trouble of a 3He counter ampliﬁer.
The resultant reliability factors obtained
from the reﬁnement were Rwp=3.32%,
Rp=2.55%, RI=1.66%, RF=0.94%, and
S=1.2787. The obtained positional parameters and isotropic thermal displacement
parameters are summarized as follows;
x=0.7609(2), z=0.6630(2), B=0.46(3) A2 for
Ca; x=0.4161(4), z=0.0975(3), B=0.16(4)A2 for Co1; x=0.4434(4), z=0.6102(3) for
Co2; x=0.1974(1), z=0.1554(1), B=0.22(1)A2 for O1; x=0.6141(1), z=0.0225(1) forO2; x=0.5309(1), z=0.7886(1) for O3;
x=0.4187(1), z=0.4279(1) for O4. The
constraints are B(Co2)=B(Co1) andB(O4)=B(O3)=B(O2)=B(O1). All the yvalues are ﬁxed at 1/4, because all the sites
are 4c sites of the space group Pnma. Lattice parameters reﬁned were a=8.7911(1)A, b=2.90398(5) A, c=10.2767(1) A, and
V=262.357(7) A3. Bondlengths were calculated using the structural parameters andresulted as follows; 1.903(4) A for Co1-O2;
1.921(2) A for Co1-O3 (× 2); 1.924(2) A
for Co1-O2 (× 2); 2.013(4) A for Co1-O1;
1.886(3) A for Co2-O4; 1.931(2) A for
Co2-O4 (× 2); 1.963(2) A for Co2-O1 (× 2);
1.988(4) A for Co2-O3. The bond valenceswere calculated from the Co-O distances.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 921- 165 -

JAEA-Review 2013-039

The values are +3.1 for the Co1 sites and+3.0 for the Co2 sites. It suggests that
holes should be doped into the Co1 siterather than the Co2 site at least in lightly
doped phases, for example, obtained by Na
substitution for the Ca site. The structuralparameters reﬁned in this work would be
utilized for ab-initio band calculation todetermine electronic structure of CaCo2O4
in near future.
References[1] M. Shizuya, M. Isobe, E. TakayamaMuromachi, J. Solid State Chem. 180 (2007)
2550.
[2] M. Isobe, M. Arai, E. TakayamaMuromachi, J. Electronic Mater., in press.
[3] F. Izumi, T. Ikeda, Sci. Forum 321-324(2000) 198.

Fig. 1. Powder neutron diffraction pattern of
CaCo2O4 for the Rietveld analysis.

1-3-23- 166 -

JAEA-Review 2013-039

1-3-24Magnetic structure study of the multi-step metamagnet CeIr3Si2
Y. Muro(A), K. Motoya(A), K. Shigetoh(B), T. Takabatake(B)(A)Department of Physics, Faculty of Science and Technology, Tokyo University of
Science,(B)ADSM, Hiroshima University
CeIr3Si2 crystallizes in the orthorhombic ErRh3Si2-type structure (Imma, No.
74), which is a derivative of the hexagonal CeCo3B2-type. The lattice parameters
are a=7.1765 A, b=9.7274 A and c=5.5971
A. The results of electrical resistivity, speciﬁc heat and magnetic susceptibility measurements reveal that CeIr3Si2 is a Kondolattice 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
study of a single-crystal CeIr3Si2 has revealed that the metamagnetic transitions
at 0.6 T and 1.2 T occurs when the magnetic ﬁeld applyed along the b-axis whilethat at 0.9 T occurs when the ﬁeld applyed along c-axis[2]. We need to obtainthe magnetic structures between each transition ﬁeld in order to study the origin
of multi-step metamagnetism of CeIr3Si2.
Thus we have been carrying out the elastic
neutron scattering of powder and singlecrystal samples.
Below T N2, we observed four magnetic
Bragg peaks at Q=(0 4/3 +-2/3) and Q=(05/3 +-1/3). 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
T N2 becomes three time as large as thoseabove T N1. The temperature dependence
of integrated intensity at Q=(0 4/3 -2/3)
and Q=(0 5/3 -1/3) display a maximum
at 2.7 K in spite of no further phase transition down to 0.5 K. At last year, we obtained that this peak behavior results fromthe long time relaxation of the magnetic
structure below T N2.

Figure 1 shows the time dependence of
the intensity for Q=(0 4/3 2/3) at 1.5 K.
We determined t=0 s when the temperaturereached 1.5 K from 10 K. The intensity increases linearly with increasing time andseems to saturate at 12 hour. This behavior indicates that the transition at T N2 isof ﬁrst order and that the frustration exists
in the magnetic interaction between Ce 4f
moments.
[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. Time dependence of the integrated intensity
at (0 4/3 2/3) when the sample is cooled from 10 K
to 1.5 K.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 932- 167 -

JAEA-Review 2013-039

1-3-25Magnetic structure of a pressure-induced magnetically ordered phase in YbAgGe
with a quasi-kagome lattice
K. Umeo1 , H. Kubo2 , T. Onimaru2 , K. Katoh3 , T. Matsumura2 , N. Aso4 and T.
Takabatake2
1 Cryogenics and Instrumental Analysis Division, N-BARD, Hiroshima Univ.,
1-3-1 Kagamiyama, Higashi-Hiroshima, 739-8526
2 Department of Quantum Matter, ADSM, Hiroshima Univ.,
1-3-1 Kagamiyama, Higashi-Hiroshima, 739-8530
3 Department of Applied Physics, National Defense Acadeny, Yokosuka, 239-8686
4 Institute for Solid State Physics, The University of Tokyo, 106-1 Shirakata, Tokai, 319-1106
loaded in an aluminum can under 10 atm
pressure of puriﬁed helium gas. It wascooled down to 35 mK with a 3 He-4 He dilution refrigerator.
Fig. 1 shows the 2θ scans at T=80 mK <TM2 (red) and 1.5 K > TM1 (green). At T=80
mK, we found magnetic Bragg reﬂections
which are indexed with k2 , whereas we obseved no magnetic reﬂection with k1 . Measurements at TM2 < T < TM1 could not be
performed, because of temperature instability due to troubles of the dilution refrigerator. We are now in progress to analyse
the data to determine the magnetic structure below TM2 by using FullProf.[5]References[1] K. Umeo et al.: J. P. S. J., 73 (2004)537.
[2] B. Fåk et al.: Physica B 378-380 (2006)669.
[3] K. Umeo et al.: Physica B 359-361 (2005)130.
[4] H. Kubo et al.: J. P. S. J., 77 (2008)023704.
[5] J. Rodriguez-Carvajal et al.: Physica B 192(1993) 55.
150
T = 80 mK
T = 1.5 K

YbAgGe powder-1ki=2.67 A
4G, 40-PG-80-S-80-PG-Open (2-axis)

2 0 0 1/3 0 4/3
4/3 -2 2/3

110-2/3 -1 1/3
1/3 1 2/3

001

100

50

1/3 1 1/3
1/3 -1 2/3

propagation vector k = [1/3, 0, 1/3]

1/3 -1 1/3
1/3 0 -2/3

100

-2/3 0 1/3

Intensity (cps)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] and TM2 =0.65
K with k2 =[1/3, 0, 1/3] .[1, 2] A tail in thespeciﬁc-heat C ( T ) extended above TM1 was
attributed to effects of magnetic frustration
inherent to the quasi-Kagome lattice of
the Yb sublattice.[1] Recently, an anomalous phase diagram of YbAgGe underpressures has been constructed from the
C ( T ) and resistivity measurements.[3, 4]
With applying pressure above 0.5 GPa, theresistivity anomalies at TM1 and TM2 merge
into a sharp drop at TM =0.85 K.[3] In thepressure range 0.5 < P < 1.5 GPa, TM (P)remains constant, while above P∗ = 1.6
GPa, TM (P) increases linearly. Concomitantly, the anomaly of C ( T ) at TM converts
from a ﬁrst-order type sharp peak to asecond-order type jump of a conventional
magnetic compound without geometricalfrustration. The magnetic entropy at TM
rises for P > P∗ , while the Kondo temperature does not change.[4] These ﬁndings
suggest that the sudden rise of TM (P) for P> P∗ is a consequence of the release of themagnetic frustration.
In the present work, in order to determine magnetic structures at ambientpressure, we performed neutron diffraction experiments. Measurements were preformed on a sample prepared by the Bridgman method. The powdered sample waswrapped in an aluminum foil, and was

Nuclear
Mag

10

20

30

40

50

2q (deg.)

Fig. 1. 2θ scans at T=80 mK and 1.5 K indicated withthe red and green curves, respectively. The red andgreen lines, respectively, are calculated angles of nuclear and magnetic reﬂections with k2 =[1/3, 0, 1/3].

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-3-26Competition between Hidden Order and Pressure-Induced Antiferromagnetism inURu2 Si2
H. Amitsuka A , Y. Ikeda A , I. Kawasaki A , S. Takayama A , D. Nishikawa A , and M.
YokoyamaB ,A Graduate School of Science, Hokkaido University, B Faculty of Science, Ibaraki University
Heavy fermion compound URu2 Si2shows an elusive phase transition at 17.5
K, whose order parameter and orderingvector have not been found yet. Kiss etal. proposed that the magnetic octupoles
could be the ‘hidden’ order parameter on
the basis of group theory and a crystal
ﬁeld model. They also predicted thatthe magnetic dipoles are coupled withthe octupoles via quadrupoles, and thus
can be induced by lowering the crystal
symmetry on U-site from tetragonal toorthorhombic [1]. This lattice distortion
can be generated by applying uniaxial
stress (σ). In this project, we performed
the elastic-neutron-scattering experimentsof URu2 Si2 under uniaxial stress to test
this prediction by seaching for the induced
dipole moments. Scattering planes (h0l)and (hhl)were chosen for the uniaxial stressσ  [100] and [110], respectively. Spectrometers GPTAS(4G) and PONTA(5G) in JAEA
were used. The uniaxial pressure devise
used were designed by Kawarazaki et al[2]. As a consequence, in the present setup
with σ applied up to ∼2 kbar, the magnetic
dipole moments were not detected, except
the antiferromagnetic moments observedat σ = 0 (Fig. 1).
[1] A. Kiss et al, Phys. Rev. B 71 (2005)
054415.
[2] S. Kawarazaki et al, Jpn. J. Appl. Phys.
41 (2002) 6252.

Fig. 1. Neutron scattering intensity observed by amesh scan in the (hhl) scattering plane for uniaxial
stress applied perpendicular to the plane.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-3-27

Quasi-elastic neutron scattering measurements on the kagome lattice
antiferromagnet KFe3 (OH)6 (SO4 )2K. Matan1 , T. J. Sato1 , D. Grohol2 , D. G. Nocera2 , and Y. S. Lee2
1 ISSP, U. of Tokyo and 2 MIT
Physics of geometrically frustrated spin
systems is unconventional due to the collective behavior of interacting electron
spins that are inﬂuenced by the topologyof the underlying lattice. One of the mostfrustrated lattices in 2 dimensions (2D) is a
kagome lattice, which is formed by cornersharing triangles. One ideal realization ofthis type of lattice is jarosite. This class ofcompounds is particular ideal for a studyof magnetic properties of the kagome lattice because (1) it consists of single layers of undistorted kagome planes, (2) it
can be synthesized with compositions thatare stoichiometrically pure, and (3) large
crystals can be mode for inelastic neutron scattering. Jarosite is composed ofkagome planes formed by magnetic Fe3+
ions with spin 5/2. These magnetic ions,which are located inside tilted octahedral
cages formed by six oxygen atoms, sit ateach corner of the corner-sharing triangles
that form the perfect kagome planes. The
kagome planes are well separated by nonmagnetic ions, making an interlayer coupling negligibly small. The system orders magnetically at TN = 65 K due to
Dzyaloshinskii-Moriya interactions and interlayer coupling. Our previous inelastic neutron scattering measurements show
well-deﬁned spin-wave excitations in theordered state with the ﬁrst observation ofa lifted zero-energy mode [1]. Above TN ,we observe spin ﬂuctuations with uniform
spin chirality [2]. In this study, we utilized
neutron scattering to investigate temperature dependence of correlation length ofspin ﬂuctuations above TN . The measurements were performed on a single crystal
sample at GPTAS (4G) with an incident energy of 14.7 meV and collimations 40-40-S40-open in a 2-axis mode, where ﬁnal energy is integrated according to quasi-elastic

approximation. Pyrolytic graphite ﬁlters
were placed in the incident beam to reduce
higher-order contamination. The sample
was cooled using a closed cycle 4He cryostat. The energy-integrated intensities of
the quasi-elastic neutron scattering above
TN were measured at Q=(1,0,0). Figure 1(a)shows a typical Q-scan around (1,0,0) measured at 66 K, slightly above TN . The intrinsic widths (correlations lengths) wereextracted by ﬁtting the data to Lorentzian
convolved with the experimental resolution functions. Temperature dependenceof correlation length is shown in Fig. 1(b),which shows the results from our measurements at HFIR, Oak Ridge National Laboratory. A solid line shows a ﬁt to theBerezinskii-Kosterlitz-Thouless (BKT) theory for 2D XY model. In summary, our preliminary neutron scattering measurements
show a signature of the BKT transition
above TN , consistent with the 2D XY universality class.
[1] K. Matan, D. Grohol, D. G. Nocera, T.
Yildirim, A. B. Harris, S.-H. Lee, S. E. Nagler, and Y. S. Lee, Phys. Rev. Lett,. 96,
247201 (2006).
[2] D. Grohol, K. Matan, J.H. Cho, S.H.
Lee, J.W. Lynn, D.G. Nocera, and Y.S. Lee,
Nature Materials, 4: 323-328 (2005)
(a)

(b)

Fig. 1. (a) A representative scan of the quasi-elastic
scattering around (1,0,0) at 66 K. A line shows a ﬁt
to a Lorentzian. (b) The log of correlation length isplotted as a function of a reduced temperature. A
line shows a ﬁt to the BKT theory.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 1004

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JAEA-Review 2013-039

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1.  ୰ ᛶᏊᩓ஘ 4 㠀ᬗ㉁㺃ᾮయ 


1. Neutron Scattering

4 Amorphous࣭Liquid- 171 -

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JAEA-Review 2013-039

1-4-1
Analogy on the Self-assembled Fractal-like Structure between the Niobate
Nanosheet Colloidal Solution and Block Copolymer Lamellar Morphology
D. Yamaguchi, N. Miyamoto1 , S. Koizumi, T. Nakato2 , S. Akasaka3 , M. I. Kim3 ,H. Hasegawa3 and T. Hashimoto
Advanced Science Research Center, Japan Atomic Energy Agency (JAEA), Tokai, Ibaraki 319-1195
1
Department of Life, Environment and Materials Science, Fukuoka Institute of Technology, 3-30-1
Wajiro-higashi Higashi-ku, Fukuoka 811-0295
2
Division of Bio-Applications and Systems Engineering (BASE), Institute of Symbiotic Science andTechnology, Tokyo University of Agriculture and Technology, 2-24-16 Naka-cho, Koganei-shi, Tokyo
184-8588
3
Department of Polymer Chemistry, Graduate School of Engineering, Kyoto University, Katsura,
Nishikyo-ku, Kyoto 615-8510

原子炉：JRR-3

装置：PNO(3G)

ent blend composition and the specimen of
50/50 mixture shows a similar mass-fractal
dimension of Dm =2.9 to that of the niobate
nanosheet specimen.
11

10

-2
-2.9
10

pure BCP(100/0)

9

10
10
-1

Intensity (cm )Introduction
In the previous study, according to theconcept of fractal we investigated the structure of an aqueous dispersion of niobate
nanosheets by the scattering method within
the wide length scales from Åto tens of μm
and characterized a fractal-like structure having a speciﬁc mass-fractal dimension of Dm=2.9 1) . We attributed this fractal-like structure to some concentration ﬂuctuations of thenanosheets, giving rise to water-rich regions,which originate from undulation of stacks ofthe nanosheets.
In this study, we further investigate thisspeciﬁc fractal-like structure of Dm =2.9
along the concept of the structural analogy
between the aqueous dispersion of niobate
nanosheets and lamellar microdomains consisting of block copolymers which are dispersed in the matrix of constituent homopolymer (what is called ”dry brush” system 2) ).
Experiment
The mixtures of block copolymer (BCP)
and constituent homopolymer (HP) were prepared on three diﬀerent compositions, that is,
BCP/HP= 70/30, 50/50 and 20/80 (w/w),
respectively. The scattering measurements
were performed on the Bonse-Hart type double crystal ultra-small-angle neutron scattering diﬀractometer(PNO) and the focusing
small-angle neutron scattering spectrometer(SANS-J-II) at the research reactor JRR-3.
From the scattering proﬁles shown in Fig.1,
we can discern that the diﬀerent mass fractal dimensions were observed at the diﬀer-

10
10
10
10

7

-2

5

blend
(70/30)3(shift +2)

1

-2.9

blend
(50/50)-1(no shift)

-3

blend
(20/80)(shift -2)

10
10
10
10

-5

nanosheet solution(3.6 vol. %)

-7

-2.9

-9

-11

10

(shift -7)

-2
-4

10

-3

-2

-1

10
10
-1
q (nm )

10

0

1

10

Figure 1: Power-law Behaviors of Niobate Nanosheet
Solution and Block Copolymer Lamellar Morphology.

References
1) D. Yamaguchi, et al. :“Hierarchical Structure of
Niobate nanosheets in Aqueous Solution”, J. Appl.
Cryst., 40, s101 (2007).
2) S. Koizumi, et al. :“Ordered Structure of Block
Polymer/Homopolymer Mixtures, 4. Vesicle Formation and Macrophase Separation”, Makromol.
Chem. Macromol Symp., 62, 75 (1992).

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JAEA-Review 2013-039

1-4-2

Hydrophobic hydration and partial molar volume of alcohol aqueous solutions
K. Maruyama(1), M. Nakada(2) and M. Misawa(3)(1)Fac. of science, Niigata University, (2) Graduate School of Sci. and Tec., Niigata Univ., (3)J-Parc center, KEK
In a previous paper [1], we reported
that the characteristic behavior of the excess partial molar volume of 1-propanolwater mixture was interpreted satisfactorily in terms of the hydrophobic hydration of the fractal surface of alcohol clusters. This results were also conﬁrmed on tbutyl alcohol-water mixtures. In this study
we investigated two other alcohol, i.e.
ethanol and 2-propanol, aqueous solutions.
By analysing the dynamic structure factors
with a relaxing cage model[2], the common
behavior of these samples were revealed.
The quasielastic neutron scattering
measurements on alcohol aqueous solutions were performed by using AGNES
spectrometer and its standard accessery.
The samples, their alcohol composition x,
and messured temperature were ethanol
x=0.0-0.25, 298, 320 and 343K; 2-propanol
x=0.0-0.17, 298, 320, and 343K. The metylgroups of alcohols were deuterized in order to investigate the diffusive propertiesof water molecules. The sample cell was analuminum double cylindrical cell with thesample thickness of 0.3 and 0.5mm. The accumurate time was 4 hours for each condition.
The dynamic structure factor S(Q,E) was
obtained by a usual process with a program
AGDAS. The statistical accuracy of S(Q,E)
was good enough for the detailed analysis. The number fraction of hydrating water molecules α was derrived by using two
states approximation and some dynamic
properties, e.g. diffusion coefﬁcient D andrelaxation time τ, were also obtained witha relaxing cage model. Fiugure 1 shows thederrived D as a fuction of α. In this ﬁgure D has a good linear dependence on α,
which means the α is a good parameter descriving the state of water molecules. Figure 1 also shows that D of all slcohol solu-

tions have nearly the same depenednce on
α, which means the dynamics of water inboth bulk and hydrating states is independent on the species of alcohol.
References[1] M. Misawa, Y. Inamura, D. Hosaka andO. Yamamuro, J. Chem. Phys., 125 (2006)
074502.
[2] A. Cunsolo, A. Orecchini, C. Petrillo,
and F. Sacchetti, J. Chem. Phys. 124 (2006)
084503.

Fig. 1. Diffusion coeﬁcient D of some alcohol aqueous solutions as a function of the number fraction ofhysrating water molecules α.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 670- 174 -

JAEA-Review 2013-039

1-4-3

Hydration structure around the nitrogen atom of the pyridine molecule
Yasuo Kameda, Asami Maki, Yuko Amo, Takeshi Usuki
Dept. Material & Biological Chemistry, Faculty of Science, Yamagata Univ.
The coordination property of the pyridinyl
nitrogen atom plays an important role in
the wide ﬁelds of chemical and biologicalsciences, however, the experimental determination of the hydration structure of thepyridine molecule has not been reported.
In the present report, we describe resultsof neutron diffraction measurements on
the aqueous 10 mol% pyridine solutions
in which 14N/15 and H/D isotopic ratios
were changed.
Neutron diffraction measurements werecarried out at 298 K using the ISSP diffractometer, 4G (GPTAS) installed at the JRR5M research reactor with an incident neutron wavelength of 1.093(3) A. Scatteredneutrons were collected over the angularrange of 3 < 2 theta <118 deg. corresponding to 0.3 < Q < 9.8 1/A. Preset timewas 180 s for each data point. After correction for the background, absorption andmultiple scattering, the observed scattering intensities were converted to the absolute scattering cross section by the use ofcorrected scattering cross section from thevanadium rod.
The ﬁrst-order difference function between [1] (14N-pyridine-D2O) and (15Npyridine-D2O) was determined from thedifference in the observed scattering crosssections between sample solutions withdifferent 14N/15N compositions. The distribution function around the pyridinyl nitrogen atom was derived by the Fouriertransform of the observed ﬁrst-order difference function (Fig. 1a). In the present
experimental condition, contributions fromthe N-O(water) and N-D(water) partial
structure factors are dominant in the observed difference function. The calculated intramolecular contribution within
the pyridine molecule was subtracted fromthe observed total difference function to
obtain the intermolecular difference func-

tion. The intermolecular distribution function was evaluated by the Fourier transform of the intermolecular difference function (Fig. 1b).
The ﬁrst peak observed in the intermolecular distribution function is assigned to thenearest neighbor N…D (water) interaction.
The least squares ﬁtting analysis of the observed intermolecular difference function
revealed that, on the average, 2.4 watermolecules are hydrogen-bonded in the N…
D-O-D type. The nearest neighbor N…D
distance is determined to be 1.93 A.
Reference[1] J. E. Enderby, G. W. Neilson, Water,
A Comprehensive Treatise , Plenum Press,
New York (1979), Vol. 6, p. 1.

Fig. 1. Fig. 1 a) Total and b) intermolecular distribution functions around nitrogen atom of the pyridine
molecule.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-4-4

DMF-induced Phase Separation of HFIP-Water Mixtures
T. Takamuku, T. Shimomura, M. Tachikawa
Saga University
At an ambient condition, 1,1,1,3,3,3hexaﬂuoro-2-propanol (HFIP) is misciblewith water at any ratio. However, themixing state of HFIP-water solutions at
a nano-scale is not homogeneous [1]. We
have been found in the previous study
that phase separation of HFIP-water solutions occurs by adding amide molecules,
such as N-methylformamide (NMF) [2].
The amide-induced phase separation of
HFIP-water mixtures occurs in a circular area of triangle phase diagram, andthe area becomes wider with increasing hydrophobicity of amide in the sequence of N-methylpropionamide (NMP)> N-methylacetamide (NMA) > NMF.
This may be due to the enhancement of
nano-heterogeneity of HFIP-water solutions arising from solvation for hydrophobic parts of amide molecules by hydrophobic HFIP clusters formed in the solutions.
In the present study, phase separation of
HFIP-water solutions by addition of N,Ndimethylformamide (DMF) has been clariﬁed by using small-angle neutron scattering (SANS) technique. A DMF molecule
cannot form N-H…O-H hydrogen bonddue to the methylation of both amino hydrogen atoms, although the carbonyl oxygen can form C=O…H-O hydrogen bond as
well as the other amide molecules.
The phase diagram of amide-induced
phase separation of HFIP-water solutions
at 298 K indicated that the circular area of
DMF-induced phase separation of HFIPwater solutions is wider than that of the
NMA system, but slightly narrower thanthat of the NMP one. According to thephase diagram, SANS experiments using
the SANS-U spectrometer have been madeon DMF-HFIP-D2O ternary solutions at
HFIP mole fraction of 0.14, which corresponds to the volume ratio of HFIP towater of 1:1, with varying DMF content.

The Ornstein-Zernike correlation lengths
Xi were estimated from SANS spectra forthe ternary solutions. Figure 1 (a) and (b)show the Xi values for all the ternary solutions below and above the circular areaof phase separation, respectively. As seenin Figure 1 (a), the Xi values for all theamide systems increase with increasing
amide content, suggesting that the nanoheterogeneity of the solutions is enhanced
when the amide content increases. The increase in the Xi with increasing amide content agrees with the fact that the amideinduced phase separation toward the lower
critical line takes place at lower amide content in the sequence of NMP = DMF <NMA < NMF. On the other hand, Figure1(b) reveals that the nano-heterogeneity ofthe solutions diminishes with lower amide
content in the sequence of NMF < NMA =DMF < NMP. This is consistent with that
one-phase solution is recovered above theupper critical line with lower amide content in the sequence. The present results
suggest that the hydrophobicity of DMF is
between those of NMA and NMP.
References[1] K. Yoshida, T. Yamaguchi, T. Adachi, T.
Otomo, D. Matsuo, T. Takamuku, and N.
Nishi, J. Chem. Phys., 119, 6132-6142 (2003).
[2] T. Takamuku, H. Wada, and K. Fujii,
Activity Reports on Neutron Scattering Research, #361, (2007).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

Fig. 1. Amide mole fraction dependence of Xi for
amide-HFIP-D2O ternary solutions (a) below and(b) above two-phase area of phase diagram.

1-4-4- 177 -

JAEA-Review 2013-039

1-4-5

Alkyl-chain Dependence of Mixing State for Methanol Solutions of
Imidazolium-based Ionic Liquids
T. Takamuku, T. Shimomura, K. Fujii
Saga University
Room temperature ionic liquids attract
much attention in various chemical ﬁelds,such as organic synthesis, extraction, andelectric device, because of their properties
of novolatility, noﬂammability, and highelectroconductivity. However, their highviscosity is a serious problem for application of ionic liquids in such ﬁelds. Thus,
ionic liquids are often utilized by mixing
them with cosolvent like water, methanol,
and acetonitrile. The microscopic state for
mixtures of ionic liquid and molecularliquid is essential to evolve the application of ionic liquids. In the present work,
the mixing state of methanol solutions ofimidazolium-based ionic liquid has been
evaluated by using small-angel neutron
scattering (SANS) technique.
1-alkyl-3-methylimidazolium bis(triﬂuoro
methanesulfonyl) amides Cnmim+TFSAwith the different length of alkyl chain ofn = 4, 6, 8, 10, and 12 were synthesized bya conventional method. Sample solutions
were prepared by mixing Cnmim+TFSAwith deuterated methanol at various
methanol mole fractions XCD3OD. SANS
spectra for the sample solutions at 298
K were measured by using the SANS-U
spectrometer with the camera lengths of 1
and 4 m.
Figure 1 shows the Ornstein-Zernikecorrelation lengths Xi for Cnmim+TFSA–
CD3OD mixtures estimated from SANS
spectra as a function of XCD3OD. The dependence of the length of alkyl chain isclearly observed in the ﬁgure. The Xi value
for the methanol mixture of C4mim+TFSAreaches a maximum at XCD3OD = 0.95
when the mole fraction increases from 0.8
to 1, suggesting that the mixing of the ionicliquid and methanol is the most inhomogeneous at XCD3OD = 0.95 among the mole
fractions examined. However, those for themethanol mixtures of Cnmim+TFSA- withn = 6-12 indicate a maximum at the higher
mole fraction of XCD3OD = 0.97. Furthermore, the maximum of Xi increases
with increasing length of the alkyl group.
The present results thus suggest that thelonger the alkyl group of imidazolium, themore the heterogeneity of the mixtures is
evolved. This is because the hydrophobic
ﬁeld is easily formed by the longer alkyl
chain and methanol molecules aggregateby hydrogen bonds in the ﬁeld.

Fig. 1. Figure 1. Xi for Cnmim+TFSA–CD3OD mixtures as a function of methanol mole fraction.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 710- 178 -

JAEA-Review 2013-039

1-4-6

Nano-scale aggregation structure formed in room temperature ionic liquid and its
application to the new reaction ﬁeld
K. Fujii (A), T. Shimomura (A), T. Takamuku (A), Y. Umebayashi (B), S. Ishiguro (B)(A) Saga University, (B) Kyushu University
Small-angle neutron scattering(SANS) experiments were made onthe
1-alkyl-3-methylimidazoliumbis(triﬂuoromethanesulfonyl)amide,[C(n)H(2n+1)mim+][TFSA-] (n: alkylchain length of the imidazolium cation)
ionic liquids containing a hydrophobic
solute such as surfactant and alcohol, andwe discussed the aggregation structureof hydrophobic solute in the ionic liquids. SANS measurements were carriedout by using SANS-U spectrometer at
298 K and the scattering intensities forthe samples were accumulated on thedetector at the camera lengths of 1 and
4 m for 10 min and 1 h, respectively. In
this work, the deuterated ionic liquids,[C(n)D(2n+1)mim+][TFSA-] where alkylchain H atoms is substituted by D atoms
were synthesized and were used as thesolvents on SANS measurements.
(1) Dodecyl-trimethylammonium bromide(DTAB) in [C(n)D(2n+1)mim+][TFSA-]
with n =2 and 4.
SANS proﬁle observed for
DTAB/[C2D5mim+][TFSA-]
solution
did not show a signiﬁcant peak to obtain a
ﬂat SANS pattern at all DTAB concentrations (C = 0 - 0.04 mol kg-1). The same wasobtained for DTAB/[C4D9mim+][TFSA-]
system. These results indicate that nanoscale structure such as DTAB micelle is
not formed in the ionic liquids. Here, it
has revealed by our density measurementthat the apparent molar volume estimatedin DTAB/[C2D5mim+][TFSA-] system
markedly increases with DTAB concentration up to ca. 0.01 mol kg-1 and is
kept a constant at C > 0.01 mol kg-1. We
concluded on the basis of SANS and molar
volume studies that DTAB molecules are
not form a nano scale micelle due to a
speciﬁc interaction between DTAB andionic liquid. It is need to elucidate theintermolecular interaction at micro scalelevel, and we are trying now large-angle
X-ray scattering and MD simulation.
(2) Alcohols, C(n)D(2n+1)OH (n = 2, 4 and6) in [C12H25mim+][TFSA-].
According to our previous SANS study, it
is established that neat [C12mim+][TFSA] shows an intense SANS peak at aroundQ = 0.2-0.3 A-1 and the peak is ascribedto the long-range TFSA-TFSA correlation in
the ionic liquid. In this study, the peak position was unchanged with adding C2D5OH
and C4D9OH, implying that liquid structure in neat [C12H25mim+][TFSA-] remains in both alcohol/IL binary systems
and the solvation of alcohol molecule
by IL is weak. On the other hand,in C6D13OH/[C12H25mim+][TFSA-] system, the peak position slightly shifts to ahigher Q-range and the intensity decreases
with C6D13OH, implying that liquid structure of neat [C12H25mim+][TFSA-] is destroyed due to hydrophobic interaction
between alkyl groups of [C12H25mim+]cation and C6D13OH to give the shifted Q
and the decrease in the SANS intensity.
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)

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JAEA-Review 2013-039

1-4-7

Temperature variation of the diﬀusional motion of water molecules in n-propyl
alcohol aqueous solution
K. Maruyama(A), M. Nakada(B), T. Kikuchi(C), C. Matsumoto(A), and O. Yamamuro(C)(A)Fac. Sci., Niigata Univ., (B) Grad. Sch., Niigata Univ., (C)ISSP-NSL Univ. Tokyo,
We carried out the quasielastic neutron scattering (QENS) measurements forn-propyl alcohol aqueous solutions, thecomposition of n-propyl alcohol xp = 0.0 to
0.167, by using High Resolution Clod Neutron Scattering Spectrometer AGNES. The
temperature range was 268 to 298 K. We
could obtain quasielastic spectra with goodresolution. Hence the experimental data forsamples are well distinguishable from theS(Q,E) of vanadium, which was used as theresolution function.
In order to get an information of diffusive dynamics of water molecules in npropyl alcohol aqueous solutions, we analysed S(Q,E)’s with relaxing cage model(RCM)[1]. The ﬁtting by RCM analysis toexperimental data was good in whole E
range. Then, we obtained diffusion coefﬁcients D of water molecules in every measured solution. The D obtained from highresolution mode measurement and RCM
analysis at 298 K shows good agreementwith the values in ref. 2. This agreement
is quantitatively better than the values forstandard mode measurement and RCM
analysis which we had carried out in previous study.

hol molecules or clusters. Thus we believethat this result relates to the behaviour ofhydrophobic hydration in alcohol aqueous
solution.
[1] M. Nakada, K. Maruyama, O. Yamamuro, and M. Misawa, J. Chem. Phys. 130(2009) 074503.
[2] E. Hawlicka, and L. A. Woolf, J. Phys.
Chem. 96 (1992) 1554.

Fig. 1. The Arrhenius plot of diffusion coefﬁcientsof water molecules in the n-propyl alcohol aqueous
solutions.

Furthermore, since we were interested
in temperature dependence of diffusive dynamics of water molecules in solutions, an
Arrhenius plot of D of water molecules isshown in Fig. 1. As seen in Fig. 1, D for thesolution of xp = 0.167 turns down around
298 K, which suggests that the diffusive dynamics of water molecules in the solutionof xp = 0.167 seems to change at this condition, and is consistent with previous result,in which we found that at the condition of
xp = 0.167 and at 298 K, the almost all watermolecules hydrophobically hydrate to alcoActivity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 780- 180 -

JAEA-Review 2013-039

1-4-8

Study on micro-solvent extraction mechanism using ionic liquid-water mixed
solvents by SANS
K. Fujii, S. Homi, T. Takamuku and M. Tabata
Saga Univevrsity
Aqueous mixed solvents of ionicliquids (ILs) were measured by smallangle neutron scattering (SANS) to
elucidate the liquid structure on nanometer scale. The aqueous IL samples
examined were prepared by weighting imidazolium based ionic liquid[Cnmim+X-, X = Cl, Br, CF3SO3,bis(triﬂuoromethansulfonyl)amide(TFSA)] with the alkyl-chain length n= 4, 8 and 12. SANS measurements werecarried out by using SANS-U spectrometerat 298 K and the scattering intensities forthe samples were accumulated on thedetector at the camera lengths of 1 and 4
m for 10 min and 1 h, respectively. Typicalresults are given below.
With regard to 1-butyl-3methylimidazolium (C4mim+) ionic liquid
system (IL concentration, m = 0 - 1 mol kg1), aqueous mixed solvents of C4mim+Cland C4mim+Br- show no scattering above
the background over the whole Q range
examined (0.01 < Q/A-1 < 0.35). On
the other hand, that of C4mim+CF3SO3shows a weak SANS proﬁle based on a
general Ornstein-Zernike function. Thisimplies that a hydrophobic IL anion suchas CF3SO3- is not easily solvated with water relative to Cl- and Br- anions, and thenthe CF3SO3- aggregates with hydrophobic
C4mim+ cation to form IL cluster.
With aqueous C8mim+Br- system, No signiﬁcant SANS proﬁle is observed for theconcentration m = 0.09 mol kg-1, whichis shown in Figure 1. The SANS intensity
increases with increasing IL concentration
up to 1 mol kg-1. Note that those for m =0.46 and 0.97 mol kg-1 fall on the straightline with a I(Q) = Qˆ-4 relationship on a
range of Q = 0.15 - 0.25 A-1, suggestingthat the ionic liquids aggregate with eachother to form the charged micelle in the so-lutions. By assuming a spherical charged
micelle, we analyzed the obtained data byusing core-shell spherical model (form factor) with a Hyter-Penforld structure factor
for charged macroions. As seen in Figure 1,
the observed I(Q) is good agreement withthe theoretical one (solid line), as the result,the core radius and shell thickness in the IL
micelle were estimated to be 14.8 and 3.3
A, respectively, for m = 0.97 mol kg-1 andthe same values were obtained for m = 0.46
mol kg-1.

Fig. 1.
SANS proﬁles observed for aqueous
C8mimBr system. The solid lines correspond to themodel ﬁt results.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 856- 181 -

JAEA-Review 2013-039

1-4-9

Structural investigation on super crtical CO2 and co-solvent system
Masaaki Sugiyama, Takashi Sato, Keiji Ito, Kazuhiro Mori and Toshiaru Fukunaga
Research Reactor Institute, Kyoto University
Supercritical carbon dioxide (sc-CO2 ) is
widely recognized as an environmentally
accepted solvent for reaction chemistry.
Unfortunately, this green solvent has lesser
solubility than the other major organic
solvents. To overcome this point, small
amount of the second chemical, entrainer(co-solvent), is added to enhance the solubility. Therefore, it is very important to understand this entrainer effect from the bothof fundamental and application chemistry.
The solvent property of sc-CO2 is deeply
related with its structure of density ﬂuctuation in nano-scale. It means that the clariﬁcation of the nanostructure is very important to understand the solvent property of sc-CO2 and that with co-solvent.
Small-angle neutron scattering (SANS) is
one of the most suitable technique to clarify the nanostructure. Because neutron hasvery high trasmission for many substances
comaped with X-ray: artiﬁcial sapphirewith the thickness of 10 mm can be used
for the window of a pressure cell. In thisstudy, we observe the SANS of sc-CO2 with
protonaed ethanol and deuterated-ethanol,and pure sc-CO2 as a reference.
SANS experiments were performed with
SANS-U spectrometer. Samples were scCO2 , sc-CO2 with 1 mol% protonatedethanol, sc-CO2 with 1 mol% deuterated
ethanol. Along the isothermal line at 39˚C,
we observed the nanostructure at 10 different density points from 0.275 g/cm3
to 0.609 g/cm3 (presuure: 7.89 MPa to
10.00 MPa, critical point of pur CO2 :31.1˚C, 0.468 g/cm3 , 7.38 MPa).
The observed SANS data were analyzed
with Ornstein-Zernike formula. The results were shown in Fig. 1. As you cansee, the peak positions of correlation lengthand density ﬂuctuation are shifted to lower
density. In the peak position, several
characteristic values, for example dissolv-

ing power, show drastical change: in thehigher density, the dissolving power becomes enhanced. Therefore, from the view
point of nanostructure, the entrainer effecthas been conﬁrmed in this study.

Fig. 1. Density dependece of observed correlationlength (a) and density ﬂuctuation (b). Open circles,
closed squares and closed circle shows those of scCO2 and sc-CO2 with 1 mol% protonated ethanol,
respectively,

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 875- 182 -

JAEA-Review 2013-039

1-4-10QENS Studies of Fast Molecular Reorientation in Isotropic, Glass, Smectic, andCrystalline Phases of 6O2OCB
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
Some of cyanobiphenyl compounds arewell known as liquid crystalline materials.
These molecules are rod-shaped consisting of two parts (rigid cyanobiphenyl
part and ﬂexible alkyl-chain part), which
is one of the keys of forming a liquid
crystalline phase. The phase behavior of
liquid crystalline material is quite sensitive
to a small change in molecular shape.
Branching modiﬁcation of the alkyl-chain
for cyanobiphenyl compounds is one ofsuch changes, which varies not only the behavior of liquid crystalline phases but also
the crystalline polymorphisms. We havebeen interested in the relation between thephase behavior and alkyl-chain motion ofsuch compounds. In the past two years,
we reported the results of the quasi-elastic
neutron scattering (QENS) measurementof (S)-4-(2-methylbutyl)-4-cyanobiphenyl(5*CB) and (S)-4-(1-methylheptyloxy)-4cyanobiphenyl (8*OCB) both of which
are the structural isomer of famous liquid crystalline materials 5CB and 8OCB
having branching structure in their alkylchains. From those investigations, it has
been revealed that the chain branchingsigniﬁcantly slows down the motion ofalkyl-chain as well as the rotational motionof whole molecule around its long axis.
This year, we report the results of QENS
measurement for another cyanobiphenyl
compound4-(2-hexyloxy-ethoxy)-4’cyanobiphenyl (6O2OCB) which is analogous to 8OCB having ?OCCO? structure in
its alkyl-chain.
Various kinds of measurements have already been made for 6O2OCB. From thecalorimetric measurements, the phase behavior of 6O2OCB has been established[1]. The isotropic liquid is easily undercooled and forms glassy state on fur-ther cooling below 218 K. There exist two
liquid crystalline phases (both of which
are metastable smectic) and two crystalline phases (metastable and stable). The
phase behavior of 6O2OCB is signiﬁcantly
different from that of 8OCB which has
two liquid crystalline phases (nematic andsmectic). The dielectric relaxation measurements have also been made, and they
showed that the molecular reorientation
around its short axis becomes quite slow
near the glass transition temperature at 218
K [1]. 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
6O2OCB using AGNES spectrometer at
JRR-3M. The measurements were madeat 370 K, 350 K, 330 K, 310K, 290 K
for isotropic liquid phase with a lowresolution mode (delta E = 120?microeV). As a spectrum of rotational motion
is approximately described by sum of adelta function (an elastic component) anda 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 thenarrow component as a diffusive motion.
The diffusion constants were obtained byusing the continuous diffusion model. An
Arrhenius plot for the diffusion constantgives the activation energy 22.1 kJ /mol
(Fig. 1). This motion may be the mixtureof the alkyl-chain tumbling motion and therotation of whole molecule around its longaxis.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 913- 183 -

JAEA-Review 2013-039

One of the interesting points is that the diffusion constant of 6O2OCB is smaller thanthat of 8OCB while it is larger than that of
8*OCB, which indicates that the ?OCCO?
structure in its alkyl-chain slows down
the chain motion less signiﬁcantly thanthe chain-branching effect. Since 6O2OCB
shows two liquid crystalline phases while
no liquid crystalline phase is found for
8*OCB, there seems some correlation between the speed of alkyl-chain motion andthe formation of liquid crystalline phase.
[1] Massalska-Arodz M., Sciesinska E., Sciesinski J., Krawczyk J., Inaba A., Zielinski P.M., Dielectric Properties of Liquid
Crystals, eds Z. Galewski, L. Sobczyk (Research Signpost Publ.); ISBN: 978-81-7895288-8 (2007) 160.

Fig. 1. Fig. 1 An Arrhenius plot of the diffusion constant for 6O2OCB, 8OCB and 8*OCB.

1-4-10- 184 -

JAEA-Review 2013-039

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1. Neutron Scattering- 185 -

5 Polymer

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JAEA-Review 2013-039

1-5-1
SANS Study of PEEK-Based Polymer Electrolyte Membrane Prepered by
Radiation-Induced Graft Polymerization
S. Hasegawa, S. Takahashi, H. Iwase1 , S. Koizumi1 and Y. Maekawa
Quantum Beam Science Directorate, JAEA, Takasaki, Gunma, 370-1292
The Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195

1

Figure 1 shows SANS results of original
PEEK substrate, grafted PEEK with a grafting degree (GD) of 46%, and PEEK-PEM
with a sulfonation degree (SD) of 90%, respectively. The SANS proﬁles of the grafted
PEEK was much larger scattering in thewhole Q-range and showed new shoulder-likepeak at around Q = 0.35 nm−1 (d = 2π/Q =13.7 nm). The d-spacing of 13.7 nm corresponds to the size of ethyl 4-styrenesulfonate
原子炉：JRR-3

装置：SANS-J(C3-2)110(1) (2) (3)

0

10
-1

SANS measurements were performed on
Focusing and polarized neutron small-angle
scattering spectrometer (SANS-J-II) at the
research reactor (JRR-3) in Japan Atomic
Energy Agency (JAEA), Tokai, Japan. The
SANS proﬁles were obtained with a sampleto-detector distances of 10 and 2.5 m, covering from Q = 0.04 to 1 nm−1 , where Q =(4π/λ) sin(θ/2) (θ and λ are the scattering
angle and the wavelength, respectively). All
SANS measurements were performed at room
temperature.

(E4S) grafts phase. The Q−2 behavior in the
Q-range of Q > 0.35 nm−1 indicated the no
sharp interface between the grafts and PEEK
substrate; namely, the E4S grafts are miscible
to the substrate PEEK chains owing to a similar hydrocarbon structures. The SANS proﬁleof the PEEK-PEM shows a similar one witha shoulder-like peak proﬁle, appeared at Q =0.38 nm−1 , which is slightly higher than thatof the grafted PEEK, i.e., smaller d = 13.2
nm. It is surprising to observe Q−2 behavior
in the Q-range of Q > 0.38 nm−1 , which also
showed the no sharp interface between thegrafts and PEEK substrate, even though thehydrolyzed PSSA grafts must be hydrophiliccompared with the E4S grafts and substrate
PEEK chains. The SANS results also showed
the 2.5 times larger size (13 nm) of ion channels consisting of poly(styrenesulfnoic acid)(PSSA) grafts than that in Naﬁon.

I(Q) (cm )Development of alternative polymer electrolyte membrane (PEM) well working under low humidity condition has been needed
to realize practical application of polymer
electrolyte fuel cells (PEFCs). Recently, byusing radiation-induced graft polymerization
technique, poly(ether ether ketone) (PEEK)based PEMs were sucessfully prepered andshowed high ion-conductivity under low humidity conditions in comparison with that for
Naﬁon. Small-angle angle neutron scattering (SANS) measurements also have been performed in order to reveal higher-order structure and morphology of these PEEK-based
PEMs, because ion-conductivity closely is related to the higher-order structure. In thisstudy, we observed morphological change of
the PEEK-based PEM during the preparation
by SANS.

-4

-1

10

-4
-2

-2

10

-3

10

2

4

6 8

2

-1

10

4

-1

6 8

Q (nm )

0

10

2

Figure 1: The SANS proﬁles of (1) original PEEK
substrate, (2) E4S-grafted PEEK with 46% GD, and(3) PEEK-PEM with 90% SD.

分野：中性子散乱（高分子）- 187 -

JAEA-Review 2013-039

1-5-2
Combined SANS, WANS, and Weighing Studies of Microbial Cellulose:
Elucidation of Hierarchical Structures in Drying Process
Y. Zhao, S. Koizumi and T. Hashimoto
Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195

We studied the structural change of the
microbial cellulose in the drying processby means of combined time-resolved measurements of small-angle neutron scattering (SANS), wide-angle neutron scattering(WANS), and weighing, as schematically illustrated in Fig.1. Combining the three Trtechniques, we are able to observe the structural change of the cellulose network in two
diﬀerent length scales on a rigorously common time scale, e.g., the changes in microscopic structure (the concentration ﬂuctuations of cellulose ﬁbrils and the air voids generated upon drying), the geometry and structure change in mesoscopic scale (the size andtotal weight of the specimen, the water concentration or hydrogen density in the scattering volume), and interrelationships between
the structural changes. We found the drying process is divided into three time regions,deﬁned by Region I, II and III. In Region I, 3dimensional shrinkage occurs and the weightloss is fast. While in Region II, only 1demensional shrinkage is observed, hence theweight loss slows down. In Region III, allchanges stop, indicating the drying process isover, however, still partial of water remains,which is believed to be bound water. Timeevolution of SANS proﬁles at representative
time during the drying process for two sample specimens in either water or heavy water is shown in Fig.2. We observe that the
microscopic structure of cellulose ﬁbrils itself,
at q-range (q denotes magnitude of scatteringvector) covered in this study, does not change
upon drying, but the amount of air voids does.
In addition, the drying ways are found to inﬂuence the size of the air voids dramaticly.
The faster the drying process is, the larger
the air voids are.

原子炉：JRR-3

装置：SANS-J(C3-2)

Figure 1: Schematic illustration of experimental setup
of time-resolved SANS, WANS and weighing measurements for the same cellulose specimen in a single
batch.

Figure 2: Time evolution of SANS proﬁles at representative times for (a) specimen 1 in water; (b) specimen
2 in heavy water during the drying process.

分野：中性子散乱（高分子）- 188 -

JAEA-Review 2013-039

1-5-3
Eﬀect of Dynamic Nuclear Polarization on Small Angle
Neutron Scatterings of Diblock Copolymer with a Lamellar Structure
Y. Noda, T. Kumada, T. Hashimoto and S. Koizumi
Advanced Science Research Center, JAEA, Tokai, Ibaraki 319-1195

We have carried out small angle neutron
scattering (SANS) measurements for 2,2,6,6tetramethylpiperidine
1-oxyl(TEMPO)
doped polymers with its proton spins polarized by a dynamic nuclear polarization(DNP) technique, in which the sample wasirradiated by a microwave with frequency of
94 GHz, at 3.3 T and 1.1 K 1) . Recently,
we applied this method to polystyrene (PS)polyisoprene (PI) diblock copolymer, inwhich TEMPO molecules selectively doped
into the PI phase by a vapor permeation
process, since the PS phase is glassy and
the PI phase is ﬂuid at the temperature of
the doping process (40 ◦ C). And the sample
with a lamellar morphology was obtainedby getting the molecular weight of the two
blocks to be close to each other. So far, there
have been no SANS study for a dynamicallypolarized sample having a lamellar structure,
although a lamellar structure can be treatedas a one-dimensional system, which allows us
a simple analysis.
As shown in Figure 1, the sample showed
a 1st, 2nd, and 3rd peaks due to the lamellar
structure. And the q value of the 1st peak (0.1nm−1 ) gave the thickness of a lamellar period
to be 63 nm. The positive polarization of P =+37 % decreased the scattering intensity by afactor of 0.04, and the negative polarization of
P = −37 % increased the scattering intensity
by a factor of 3.4. The P dependence of thescattering intensity agreed well with that of
the contrast factor calculated with assuming
P to be homogeneous through the sample. In
the calculation, we used the two phases’ massdensity, atomic composition, and polarization
determined by 1 H-NMR measurements. From
this result, it was shown that the sample waspolarized almost homogeneously.
On the other hand, at P = −37 %, therelative peak height of 2nd/1st increased to
原子炉：JRR-3

装置：SANS-J(C3-2)

twice as that at P = 0 %. This result can be
explained by the small deviation from the homogeneous P distribution; at the PI phase |P |is homogeneous (38 %), and at the PS phase|P | decreases down to 36 % as being far fromthe interface with neighboring PS phases 2) .
The successful observation of the quite small
P inhomogeneity through SANS proﬁle wasowing to the sharp peaks from the lamellar
structure with a high periodicity and thickness uniformity.

Figure 1: SANS proﬁle of the PSPI block copolymer
at the unpolarized and dynamically polarized states.

References
1) Y. Noda, T. Kumada, T. Hashimoto and S. Koizumi:“Physica B”, in press.
2) Y. Noda, T. Kumada, T. Hashimoto and S. Koizumi:“J. Appl. Crystallogr.”, in preparation.

分野：中性子散乱（高分子）- 189 -

JAEA-Review 2013-039

1-5-4

Gel structure with excess water in a surfactant solution
Youhei Kawabata,Akimi Matsuno,Tomoaki Shinoda,Tadashi Kato
Tokyo Metropolitan University
In a binary system consisting of surfactant and water, a hydrated solid phase
is formed below the Kraft temperature,
where the hydrophobic tails extend to thelength with all trans. Figure 1 shows theT-φ phase diagram of a non-ionic surfactant C16 E7 (C16 H33 (OC2 H4 )7 OH) and water system. As shown in Fig. 1, the hydrated solid phase is a two-phase coexistence of excess water and lamellar structure Lβ of bilayers whose hydrophilic tails
aresolid-likegel and interdigitated.
The hydrated solid phase is strongly turbid and has a viscoelastic property, which
is applied in cosmetic industry and so on.
So far, we have investigated the structural formation of the hydrated solid phasein the C16 E6 /water and C16 E7 /water system by means of small angle X-ray scattering (SAXS) and optical microscope. Even
though those surfactants are slightly different from each other in the head length, we
found clearly different structures in nm ∼μm scale. In μm scale observation using
optical microscope, vesicle structures andworm-like lamellar domains are observedin the C16 E7 system and C16 E6 system, respectively. The SAXS experiments showedthat the formation processes of membranes
are different between the both system. The
hydrophobic parts of surfactants hinder extends of the hydrophilic tails of the C16 E7
system, while those of the the C16 E6 system tend to extend to the full length. In
this report, we compare the dynamic andstatic structures of the C16 E7 system withthose of the C16 E6 system by using the results obtained from the SANS and NSE experiments.
The SANS experiments were carried out
using the SANS-U spectrometer. The momentum transfer q ranged over 0.003 ≤q ≤ 0.2 Å−1 . The NSE experiments were
performed using the iNSE spectrometer.

The observed range of momentum transfer
q and Fourier time t, were 0.09 ≤ q ≤ 0.15
Å−1 and 0.15 ≤ t ≤ 15 ns, respectively.
Temperature was set to 8 ◦ C for the C16 E7
system, and to 20 ◦ C for the C16 E6 system. The concentration of C16 E7 and C16 E6
is 10 wt.%, respectively. For the NSE experiments, we started the experiments after
waiting 1 hour from setting each sample tothe sample cell holder because the sample
structures should be stable.
In order to investigate the head and taillength of surfactants, we analyzed those
proﬁles using the form factor of bilayers
taking the hydration of hydrophilic parts
into account. Figure 2 indicates the time
evolutions of the length of hydrophilic tails
in each system after the temperature jump,which are obtained from the SAXS experiments. The results obtained from SANS
experiments are consistent with those obtained from SAXS experiments. We conﬁrmed that the hydrophilic tails of the
C16 E7 system are hindered from extending
to the full length around ∼ 2000sec. Figure
3 shows the universal plot of the intermediate correlation functions obtained from the
NSE experiments. If the NSE results obey
the theory proposed by Zilman and Granek[1], these plots should be straight lines. The
solid lines in Fig. 3 are the ﬁtting results byusing Zilman and Granek model. From thisanalysis, we found that the bending modulus κ of bilayers in the C16 E7 system is∼ kB T, while that in the C16 E6 system is∼ 10kB T. This indicates that the bilayersof the C16 E7 system are ﬂexible because thetail length becomes short, while those of
the C16 E6 system are rigid because the tails
tend to extend to the full length.
References[1] A. G. Zilman and R. Granek, Phys. Rev.
Lett., 77, 4788 (1996).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 351- 190 -

JAEA-Review 2013-039

Fig. 1. Figure 1 : Phase diagram of C16E7-water system. Figure 2 : The time evolution of hydrophilic
tail length. Figure 3 : Universal plot of the intermediate correlation function.

1-5-4- 191 -

JAEA-Review 2013-039

1-5-5

Structure characterization of Tetra-PEG gel having homogeneous network
structure
Takamasa Sakai(A), Takuro Matsunaga(B), Mitsuhiro Shibayama(B), Ung-il Chung(A)(A)Dep. of Bioeng, Univ. of Tokyo, (B)ISSP, Univ. of Tokyo
stoichiometric composition leads to formation of defects in the polymer chain network and results in a signiﬁcant depression of the mechanical properties. Structural models of macromer solutions and of
Tetra-PEG gels, which account for the advanced mechanical properties of Tetra-PEG
gels, are proposed.
Tetra-PEG gel-10k
OZ fit010I(q) [cm-1]

The structure of Tetra-PEG gel, a new classof biocompatible, easy-made, and highstrength hydrogels consisting of a four-arm
polyethylene glycol (PEG) network, hasbeen investigated by means of small-angle
neutron scattering (SANS). Since the TetraPEG gel is prepared by cross-end-coupling
two kinds of four-arm PEG macromers
having different functional groups at theends, i.e., amine group and succinimidyl
ester group respectively, coupling reaction
occurs exclusively between PEG chains carrying different functional groups. Structure
analyses of Tetra-PEG gels were carriedout by means of swelling experiments andSANS, and the results were discussed bytaking into account the mechanical properties of the same systems. The following
facts were disclosed.
(1) Tetra-PEG gels are stoichiometrically
prepared irrespective of the initial polymer concentration, and their swelling behaviors are well predicted by the FloryRehner theory. (2) The mechanical moduli
of Tetra-PEG gels, E and G, are proportional to the initial polymer concentrationand is one order of magnitude larger thanthe corresponding gels made with similar
tetra-arm PEG gels prepared with a lowmolecular-weight coupling reagent. This
indicates that cross-end-coupling of A- andB-type tetra-PEG is essential for gel preparation with extremely low defects. (3) The
scattering functions of the macromers canbe well reproduced by the scattering function for star polymers. (4) SANS functionsof Tetra-PEG gels can be described by simple Ornstein-Zernike function without excess scattering component originating fromcross-linking inhomogeneities. This meansthat Tetra-PEG gels are extremely homogeneous, and an ideal network free fromdefects is formed. (5) Preparation in non-

10-1

10-2

10-3

star polymer fit
0.00443 (5 mg/mL)
0.00886 (10 mg/mL)
OZ fit0.0133 (15 mg/mL)
0.0177 (20 mg/mL)
0.0354 (40 mg/mL)
0.0531 (60 mg/mL)
0.0709 (80 mg/mL)
0.0886 (100 mg/mL)
0.106 (120 mg/mL)
0.124 (140 mg/mL)
0.142 (160 mg/mL)

10-2

q [Å-1]

10-1

Fig. 1. SANS intensity functions of Tetra-PEG
gel. The solid and dashed lines are ﬁtting results of Ornstein-Zernike function for gels at highmacromer concentration and 4-arm star polymer forimperfect gels prepared at low macromer concentrations, respectively.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 681- 192 -

JAEA-Review 2013-039

1-5-6

Dispersion Stability of Carbon Black Suspensions by the Addition of Polymers
Masami Kawaguchi, Hiroki Mizukawa, and Yoshiaki Takahashi
Mie University, Kyushu University
In order to conﬁrm changes in the aggregates in the carbon black suspensions
dispersed in Naﬁon solutions under shear
ﬂow, an experiment using a rheometerbase shear ﬂow apparatus for a small angle
neutron scattering SANS-U instrument ofInstitute for Solid State Physics, the University of Tokyo at JAERI Tokai has been performed as functions of the scattering vector and the shear rate at the carbon black
concentrations of 5.0 wt and 8.0 wt % andthe ambient temperature. Naﬁon was adsorbed on the carbon black surfaces and it
played a role in the stabilization of carbon
black suspensions. After sedimentation of
the carbon black suspensions, whose surfaces were covered by adsorbed Naﬁonusing a centrifuge, the sedimented carbon black suspensions were washed several times to remove free Naﬁon chains by
the dispersion media and the re-dispersed
carbon black suspensions were obtained.
The neutron scattering intensities of the redispersed carbon black suspensions clearly
depended on the shear rate. However,
it is noticed that the scattering patterns
show two power-law regimes, irrespectiveof the shear rate: At at low q, a weakslope of ?2.3 corresponds to a mass fractal regime, whereas at high q, a power
law ?3.6 is observed for the surface fractalof the primary particle. This means thatthe basic fractal structures of the carbon
black suspensions are maintained even under shear ﬂow. Moreover, changes in theneutron scattering intensities with an increase in the shear rate are well correlatedwith the shear ﬂow behavior of the corresponding carbon black suspension. Therefore, for the ﬁrst shear thinning regions andthe plateau shear viscosity regions at theshear rates less than 50 s-1 the neutron scattering intensity rapidly decreases and attains the minimum due to the partial break-ing down the aggregated structures of the
carbon black suspensions under shear ﬂow,
whereas for the second shear thinning regions with an increase in the shear rate
beyond at the shear rate of 50 s-1 thecorresponding neutron scattering intensity
grows up and approaches to a constantvalue above at the shear rate of 200 s-1
due to the formation of some newly ordered structures of the partial ruptured carbon black suspensions under higher shear
ﬂow. Thus, changes in the neutron scattering intensities seem to be well correlatedwith changes in the structures in the carbon
black suspensions under shear ﬂow.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 693- 193 -

JAEA-Review 2013-039

1-5-7

Study on Structural Nonuniformity of Cross-linked Natural Rubber
Y. Ikeda(A), N. Higashitani(A), H. Asai(A), Y. Kokubo(A), T. Suzuki(B), N. Osaka(B), H.
Endo(B), M. Shibayama(B), and S. Kohjiya(C)(A)Dept. Chem. Mater. Technol., Kyoto Inst. Tech., (B)ISSP-NSL, Univ. Tokyo, (C)Fac. Sci.,
Mahidol Univ.
Natural rubber (NR) is one of the most important industrial materials among manypolymeric ones. Generally, NR products
are prepared by cross-linking reaction, andthe network has been thought to give characteristic properties as rubber materials.
However, it is difﬁcult to elucidate themicroscopic structure of cross-linked NR
due to non-rubber components in NR suchas proteins and lipids [1]. In this study,
we applied small-angle neutron scattering(SANS) experiments by varying a deuterated toluene (D-toluene) fraction in solvents in order to investigate the network
inhomogeneity of cross-linked NR. Twoperoxide cross-linked NR samples with different network-chain densities (SP-NR-P1
and SP-NR-P2) and uncross-linked NR (NRmilled) were subjected to the SANS experiments. Dicumyl peroxide (DCP) was used
as a cross-linking reagent. The measurements were performed at SANS-U diffractometer of Institute for Solid State Physics,
the University of Tokyo. For a contrast
matching technique, matching point of NR
was determined to be ca. 15 vol% Dtoluene fraction in a mixture of D- and Htoluene as shown in Fig.1. However, thisresult can not be utilized to delete an excess scattering from the non-rubber components due to similar scattering lengthdensities between the components andpoly(isoprene). Increase of DCP decreased
scattering intensities in the solvents whose
fractions of D-toluene were over 0.3 asshown in Fig.1(b). Contrast variation SANS
technique, on the other hand, qualitatively
suggested that a network inhomogeneity
decreased with an increase of DCP, i.e.,
network-chain density, when a scattering
length density of proteins was assumed tobe 1.8e10 cm-2.

Reference : [1] T. Karino et al., Biomacromolecules, 8, 693(2007).

Fig. 1. Fig.1 (a) SANS proﬁles of uncross-linked NR
in toluene with various D-toluene contents, (b) Effect of D-toluene fraction on scattering intensity at q
= 0.004 angstrom for three samples.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 703- 194 -

JAEA-Review 2013-039

1-5-8

Structure and compressibility of worm-like lamellar domain in a hydrated solid
phase
Youhei Kawabata1 ,Tomoaki Shinoda1 ,Yuko Nagai2 , Akira Murakami1 and Tadashi
Kato1
Tokyo Metropolitan University1 , Kao Corp.2
In a binary system consisting of surfactant and water, a hydrated solid phase
is formed below the Kraft temperature,
where the hydrophobic tails extend to thelength with all trans. The hydrated solid
phase is a two-phase coexistence of excess water and lamellar structure Lβ of bilayers whose hydrophilic tails are solidgel and interdigitated.
So far,like
we have investigated the structural formation of the hydrated solid phase in
the C16 E6 /water and C16 E7 /water system[C16 H33 (OC2 H4 )6,7 OH] by means of small
angle X-ray and neutron scattering (SAXS,SANS) and optical microscope. We foundclearly different structures in nm ∼ μm
scale, even though those surfactants areslightly different from each other in the hydrophilic segment length. Figure 1a shows
vesicle structures and worm-like lamellar domains observed in the C16 E7 system
and C16 E6 system, respectively. In thisstudy, to clarify the formation process of
the lamellar domains, we performed SANS
experiments. Especially here, we report
the hyper-swollen lamellar structure in the
C16 E7 system.
The SANS experiments were carried out
using the SANS-U spectrometer. The momentum transfer q ranged over 0.003 ≤q ≤ 0.2 Å−1 . The Krafft temperatures are
287 K for the C16 E7 system. Temperature
was jumped from 289 K to 277 ∼ 287 K.
The concentration of C16 E7 is 10 wt %, respectively.
Figure 1b shows a typical SANS proﬁle obtained at 279 K in the C16 E7 system
at about 1 hour after temperature quench.
Bragg peaks can be clearly seen, and theycorrespond to a swollen lamellar structure
whose repeat distance is 84 nm. These
Bragg peaks in such a low-Q region only

appear below 279 K and at least above 281
K, they never appear. Coincidentally, fromthe microscope experiments, we found that
below 279 K, small pieces of lamellar domains as shown in the inset of Figure 1b
coexist for a few hours. It has been considered that lamellar domains hardly fuseeach other because of the low temperatureand they become quasi-equilibrium state.
From all evidences, at present, we conclude
that this hyper-swollen lamellar structure
might be related to those small pieces oflamellar domains.

Fig. 1. The SANS proﬁle obtained at 279 K in the
C16 E7 /water system. A swollen lamellar structures
whose repeat distance is 80 nm is formed.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 723- 195 -

JAEA-Review 2013-039

1-5-9

Shear-induced onion formation of complex bilayer membrane systems
Shuji Fujii(A), Yohei Kawabata(B), and Yoshiaki Takahashi(C)(A)Nagaoka University of Technology, (B)Tokyo Metropolitan University, (C) Kyushu
University
The inﬂuence of a triblock copolymer,
poly(ethylene oxide)m-b-poly(propyleneoxide)n-b-poly(ethylene oxide)m (Pluronic
series with different PEO and PPO chain
length) on the phase behavior and on
the shear induced onion formation in thelyotropic lamellar phase of the nonionicsurfactant C10E3 was investigated bymeans of rheology, small angle neutron
scattering (SANS) and small angle lightscattering (SALS). At quiescent state,added triblock copolymer signiﬁcantly
shifted the La-L3 phase transition to lower
temperatures. Under shear, the onion
structure was not stable and easily transformed back into the lamellar phase withincreasing polymer concentration and withincreasing the polymer chain length, bothof m and n. As a typical example of theresults we obtained, polymer chain length
dependence of the time development of
2D-SANS pattern in the shear-induced
lamellar-to-onion formation process isshown in ﬁgure 1. Here, only the resultson the PPO chain length dependence areshown. At short time region, anisotropic
SANS pattern with the Bragg peak in theneutral direction, which was a representative for the parallel oriented lamellae
along the ﬂow direction, was observedfor every samples. As PPO chain length,
m, of triblock copolymer was increased,
however, the time development of theonion formation process was remarkably
affected. Samples with short PPO chain
length showed an isotropic SANS pattern,which is a signal of the onion formation.
As the PPO chain length was increased,
the isotropic SANS pattern, i.e., the onion
formation, was remarkably prohibited, andthe sample with the longest PPO chain,
m=69, showed no onion formation but theparallel oriented lamellar phase. In the rhe-

ology measurements, we found an increaseof the critical shear rate for the onset ofthe shear-thickening, which also indicatesthe instability of onion in the presenceof the triblock copolymer. Suppression of
the shear-induced onion formation might
be attributed to the enhancement of theeffective surface tension, which might bealso inﬂuenced by added triblock copolymer. These results clearly indicate that not
only the hydrophilic polymer chain, PEO,
but also the hydrophobic polymer chain,
PPO, inﬂuences the dynamic properties ofthe lamellar membranes, which would becontrolled by a combination of hydrophilic
and hydrophobic chain length. To makeclear the effect of guest components on theshear-induced nonequilibrium phenomena, it is necessary to perform experimentswith different series of complex lamellar
phase and elaborate analysis of structureon the basis of SANS.

Fig. 1. Hydrophobic polymer chain length dependence of the time development of 2D-SANS patterns for complex lamellar phase in the onion formation process. Polymer mole fraction was ﬁxed at
1mol%. Shear rate was ﬁxed at 10s-1.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 724- 196 -

JAEA-Review 2013-039

1-5-10

Small Angle Neutron Scattering Study on Metal-containing Gels Composed of
Co(II) Ion and Oligopyridines
Jun Yoshida, Shin-ichi Nishikiori, Takuro Matsunaga, Mitsuhiro Shibayama
Graduate School of Arts and Sciences, The University of Tokyo; Institute for Solid State Physics,
The University of Tokyo
In recent years, supramolecular gels composed of metal ions and organic ligands are attracting great attentions. Metalcontaining gels (metallogels) have a potential to be responsive to external stimuli
such as magnetic and electric ones so thatthey can exhibit unique properties among
the gels. However, metallogels are still minor due to their synthetic and analytic difﬁculties.
We recently found that the combinationof oligopyridines (L1 and L2) with CoCl2,
Co(NO3)2, or AgBF4 forms gels easily(Fig.
1). The formation of these gels depended
on the M(metal ion)/L(oligopyridine ligand) ratio. In every case, no gel was formedin low M/L conditions, while gelation occurred with increasing the M/L ratio. Dynamic light scattering (DLS) study for thesolutions containing the metal ions and theligands conﬁrmed that the metal ions wereeffective in forming the supramolecular
type metallogel and the solutions showed
more gel-like behavior with an increase in
the M/L ratio. However, at a certain M/Lratio, it abruptly turned into a sol state. The
details of this change could not be traced
by DLS and other spectroscopic methods.
To obtain more information about this phenomenon, we used SANS technique, which
is applicable to samples even in the solstate.
SANS intensity proﬁles for CoCl2-L1 areshown in Fig.1. In a low q region, the slopesof the proﬁles for the samples in the gelstate (M/L = 1/10, 1/4, 1/2 and 1/1) were
almost -4, while those for the samples inthe sol state (M/L = 1.5/1, 2/1) were close
to -1. These two proﬁle types correspondto the gel and the sol state, and they indicate that the sol-gel transition is accompanied by some structural change. Althougha model for the gel state is under investigation at the present stage, the proﬁles forthe sol samples could be analyzed based ona model where rods with a large aspect ratio(length >> diameter) are randomly oriented. The diameters for the samples in the
M/L ratio of 1.5/1 and 2/1 were evaluatedto be 6.8 and 10.2 nm, respectively.

Fig. 1. Gel formation from oligopyridines (L1, L2)
and metal salts, and SANS intensity proﬁles for the
combination of L1 and CoCl2

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 725- 197 -

JAEA-Review 2013-039

1-5-11

Breathing Mode in Polymer Micelles and Second Virial CoeﬃcientK. Kawashima (a), T. Kanaya (a), G. Matsuba (a), H. Endo(b)(a) ICR, Kyoto University, (b) ISSP, University of Tokyo
When diblock or triblock copolymers areadded to a selective solvent, they aggregate into spherical micelles consisting of
an inner core of insoluble blocks and anouter corona of soluble blocks, similar to
micellization of surfactants. In previous
papers [J. Chem. Phys. Solids, 60, 1367-1369(1999) , J. Chem. Phys., 122, 144905 (2005)]
we have investigated dynamics of micelles of deuterated styrene-protonated butadiene diblock copolymers (PSD-PB) anddeuterated styrene-protonated isoprene diblock copolymers (PSD-PI) in deuterated
n-decane, focusing on the chain dynamics in the corona using neutron spin echo(NSE). We observed the collective breathing mode for PSD-PI. On the other hand,
it disappeared but the Zimm mode (single chain motion) was observed for PSD-PI
although the molecular weight of PSD-PB
and PSD-PI were almost identical. This has
been assigned to the difference of the second virial coefﬁcient (A 2) between PB and
PI in deuterated n-decane. In this work wehave studied the second virial coefﬁcientand the dynamic crossover from a cooperative motion (gel mode) to a single chain
motion (the Zimm mode) to elucidate why
the collective breathing mode disappears in
the DPS-PB micelles.
We used PB with Mw=22600 and
Mw/Mn=1.05 and PI with Mw=24500,
Mw/Mn=1.06. The solvent was deuterated
n-decane. Small-angle neutron scatteringand neutron spin echo measurements weredone using SANS-U spectrometer andiNSE spectrometers in JRR-3 reactor, Tokai.
First we have evaluated the second virial
coefﬁcient A 2 of PB and PI to ﬁnd that A 2of PB is smaller than that PI, showing theinteractions among PBs are smaller thanthose among PI. We have also performed
NSE measurements on the 20 wt % PB andPI solutions. The decays of intermediate
scattering functions I(Q,t) were analyzed toevaluate the ﬁrst cumulant G. Dividing theﬁrst cumulant G by Qˆ2, we plotted G /Qˆ2
as a function of Q in Figure 1. In the high Q
region the ﬁrst cumulant is proportional toQˆ3, suggesting that the mode we observedis the Zimm mode. On the other hand, inthe low Q range G is proportional to Qˆ2.
It shows that the collective gel mode isdominant in this Q range. What we haveto emphasize is that the crossover Q fromthe Zimm mode to the gel mode depends
on sorts of polymers. The crossover Q of
PI is located to the higher value than thatof PB, showing that PI has longer-range(stronger) interaction and the collective
dynamics arises in PI in the more local
region than PB. This must be a reason why
the collective breathing mode disappearedin PSD-PB micelles.

Fig. 1. Figure 1. Q dependence of G /Qˆ2 fpr PB
and PI.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 728- 198 -

JAEA-Review 2013-039

1-5-12Distribution of Glass Transition Temperature Tg in a Polymer Thin Film by
Neutron Reﬂectivity
K. Kawashima (a), T. Kanaya (a), G. Matsuba (a), K. Nishida (a), M. Hino (b)(a) ICR, Kyoto University, (b) RRI, Kyoto University
Recent extensive studies on polymer thinﬁlms have revealed very interesting but unusual properties of polymer thin ﬁlms. It
was reported that the glass transition temperature Tg of polystyrene thin ﬁlms supported on silicon substrate decreases withdecreasing thickness below 40 nm. Similar
results were reported by many researchers
on Tg of polystyrene thin ﬁlms supported
on silicon substrate. These results were explained in terms of multi-layer structure
consisting of surface mobile layer, middle bulk-like layer and interfacial immobile layer near the substrate. It is now believed that revealing the multi-layer structure is essential to understand the unusual
properties. This has been already pointed
out by de Gennes [2000, Eur. Phys. J. E 2201], and he mentioned that further experiments should not aim at the determination of a single Tg, but at a distribution ofTg s. In this report we have studied the
distribution of glass transition temperature
Tg in a three-layer polystyrene thin ﬁlm by
neutron reﬂectivity, aiming to elucidate themulti-layer structure of polymer thin ﬁlms.
For neutron reﬂectivity (NR) measurements we used deuterated polystyrene (dPS) and hydrogenated polystyrene (h-PS)
with molecular weight Mw = 7.31 x 10ˆ5and Mw = 7.69 x 10ˆ5, and molecularweight distributions were Mw/Mn = 1.18
and 1.08, respectively. The bulk glass transition temperatures Tg of h-PS and d-PS are
100 C and 103 C, respectively. NR measurements were performed using MINE spectrometer at JRR-3 reactor in Tokai.
Figure 1 shows neutron reﬂectivity proﬁlesfrom the three-layer thin ﬁlm at 30, 60, 85
and 110 C. It is very clear that the reﬂectivity proﬁles gradually shifts to lower qwith increasing the temperature, showing
thermal expansion of the ﬁlm. The tem-

perature dependence of the total ﬁlm thickness is shown for the total ﬁlm thickness,
the top (surface), the middle and the bottom layers are shown in Figures 2(a), (b),(c) and (d), respectively. The surface layer
increases in thickness with the thermal expansivity of ˜1.3 x 10ˆ-4 Kˆ-1, which is close
to the expected value (= 1.1 x 10ˆ-4 Kˆ-1), while it begins to increase above ˜85 K
more steeply, showing that the glass transition temperature of the surface layer is
˜18 K lower than the bulk Tg. The middle layer shows a very similar thermal expnsivity in the glassy state with the top
layer, but the glass transition temperatureis ˜105 K which is very close to or little bit
higher than the bulk Tg. The middle layer
behaves as the bulk layer. On the other
hand, the bottom layer shows very different temperature dependence of the thickness from other layers. The ﬁlm thickness
is almost independent of temperature below ˜130 C, suggesting that the glass transition temperature of the bottom layer mustbe higher than 130 C. The present results
clearly show that the thin ﬁlm has a distribution of Tg.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 729- 199 -

JAEA-Review 2013-039

Fig. 1. (I) Neutron reﬂectivity proﬁles of three-layer
polystyrene thin ﬁlm. (II) Temperature dependenceof ﬁlm thickness. (a) total, (b) top layer, (c) middle
layer, (d) bottom layer.

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1-5-13

Role of Low Mw Components in Polymer Crystallization under Shear Flow
C. Ito, G. Matsuba, K. Nishida, T. Kanaya
ICR, Kyoto University
It is well known that when polymers inmelts and solutions are crystallized under elongational and/or shear ﬂows theso-called shish-kebab structure is formed,
which consists of long central ﬁber core(shish) surrounded by lamellar crystalline
structure (kebab) periodically attachedalong the shish. In the previous research,
it was found that high molecular weightcomponent composed mainly shish structure. Now, we carried out the structuralformation processes of shish-kebab during
drawing was conﬁrmed by in-situ smallangle neutron scattering (SANS) measurements on a polyethylene (PE) blend of
low molecular weight deuterated PE andhigh molecular weight hydrogenated PE(3wt%). Time-resolved SANS measurements
were performed with SANS-U spectrometer at the JRR-3M reactor in JAPAN Atomic
Energy Research Institute (JAERI), Tokai.

ing . Such disappear of kebab structure
could be caused by shish-formation process from kebab structure.
Furthermore, we evaluated the detailed
shish-kebab structure from these 2D SANS
proﬁles. The shish kebab structure can be
described as core-shell cylinder model. The
radius of core cylinder was about 45 nm
and the shell cylinder had two core cylinders.

Fig. 1. Time evolution of 2D SANS patterns during
crystallization process of PE at 110 C, drawing rate
= 6 micron/ s

On drawing process of the blends, it wasobserved that the isotropic crystal structure
gradually formed the anisotropic shishkebab structure with in-situ SANS measurements in Figure 1. At ﬁrst 10 min, theisotropic pattern changed horizontally long
ellipsoid-like proﬁles. This suggested thatthe isotropic lamella was stretched and distorted. Between 20 min and 80 min, theshish-kebab formation processes were observed. In high temperature condition, thelong spacing period increased with drawing process, while the long spacing period
decreases in low temperature condition.
In high temperature, the tie chain between lamella could extend and be pulled
off from lamella crystal because of high mobility. On the other hand, low mobility
in low temperature prevented the pulled
off process and then the lamella crystal
could be broken. After 80 min, we observed the processes of kebab evaporatActivity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 730- 201 -

JAEA-Review 2013-039

1-5-14

Neutron Scattering Study on Miscibility of Statistical Copolymer / Homopolymer
BlendsSiti Sarah A. R., D. Kawaguchi, Y. Matsushita
Dept.Appl. Chem., Nagoya Univ.
We have recently found that 4-substituted
polystyrene derivatives and polyisoprene(I) are weakly interacted and likely to
be miscible with each other. Amongthe various combinations, poly(4-tertbutylstyrene) (B) and I exhibit a lower
critical solution temperature (LCST)
type phase diagram, while poly(4-tertbutoxystyrene) (O)/I blend shows anupper critical solution temperature (UCST)
type one. Hence, competition between two
interactions having opposite temperaturedependence is expected when a copolymer
consists of B and O is blended with I. The
objective of this study is to investigate
the phase behavior of statistical copolymers composed of B and O, abbreviatedas s-BO, with I by optical microscopic(OM) observation and small-angle neutron
scattering (SANS) measurements. Several
blends of s-BOs having mol fraction of B,
mB, comparable to 0.50, with I showedboth UCST and LCST type phase diagram.
Furthermore, UCST type phase behavior
was observed for blends having small
mB, while LCST type one was for that oflarge mB at all employed temperatures.
These results imply that the attractive
interaction of B/I leads to miscibility
and that the repulsive interaction of O/I
induces immiscibility of the blends within
the temperature range studied. Hence,the phase behavior of s-BO/I blend canbe understood as a result of the competition of two interactions having opposite
temperature dependence.
To elucidate the interaction between blend
components indirectly from SANS data,
the structure factors at q=0, S(0)s, whichcorrespond to the thermodynamic susceptibility were determined by using theOrnstein-Zernike equation. S(0)s were obtained from the ﬁttings of inverse S(q) vs.

qˆ2 data to Ornstein-Zernike equation. Figure 1 gives the relation between inverse
S(0) and inverse temperature, for s-BO/dI blends together with those for O/d-I
and B/d-I blends for comparison. The inverse S(0) for O/d-I blend in Figure 1(a)decreased with a decrease in inverse T,
whereas that for B/d-I blends increased
with inverse T as shown in Figure 1(e).
This shows that the interaction of O/d-I
becomes less repulsive as temperature becomes higher and vice versa for the interaction of B/d-I. Hence, these results indicatethat O/d-I blend shows an UCST and B/dI blend has a LCST type phase behavior.
Figure 1(b) for s-BO35/d-I blend showed
qualitatively the same trend as that O/dI, however, the temperature dependenceof the inverse S(0) for s-BO/d-I blends
changed dramatically when mB reaches
to 0.49 as shown in Figure 1(c). Namely,
the inverse S(0) ﬁrst increased, but went
through a maximum at 170 °C and thenturned to decrease. This implies that sBO49/d-I blend shows both UCST and
LCST type phase behavior. Furthermore,
as mB goes up more, opposite temperature dependence was observed as shownin Figure 1(d) for s-BO66/d-I blends. The
inverse S(0) increased with decreasing inverse T, indicating LCST behavior which
is similar to B/d-I blend. These results revealed by SANS experiments for s-BO/dI blends are in good accordance with OM
observation. Thus, we were able to displaythat the phase behavior of s-BO/d-I blends
change from UCST to LCST type one withan increase in mB due to the competitionof B/I and O/I opposite interactions andshow both UCST and LCST type phase behavior at balanced condition.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 741- 202 -

JAEA-Review 2013-039

Fig. 1. Temperature dependence of the inverse S(0)of (a) O/d-I, (b) s-BO35/d-I, (c) s-BO49/d-I, (d) sBO66/d-I and (e) B/d-I blends.

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JAEA-Review 2013-039

1-5-15

Dynamical Properties of Nanoporous Structure in Syndiotactic Polystyrene
Fumitoshi Kaneko, Tatsuya Kawaguchi, Kenji Okuyama
Graduate School of Science, Osaka University
Syndiotactic polystyrene (sPS) is a relatively new commodity polymer, which exhibits a variety of crystalline states. The
δe phase of sPS occupies a unique position
from the viewpoints of structure chemistryof polymers. In the δe phase, there exist
two relatively large cavities between sPS
helices taking TTGG conformation. Eachcavities has a volume of nearly 120A3 . Thisnanoporus structure is regarded as the ﬁrst
example of molecular sieve in polymericmaterials. Unlike the ordinary crystalline
states of polymers, the density of the δephase (0.977 g cm−3 ) is less than that of theamorphous state (1.05 g cm−3 ). It seems
that this unique structure exerts a considerable inﬂuence on the dynamical propertiesof the δe phase.
In this study, we compared the QNS
spectrum of the δe phase with that of theγ phase and the glass state of sPS. In theγ phase, sPS helices takes TTGG conformation like those of the δe phase but they aremuch more densely packed. All QNS spectra were measured with AGNES spectrometer of JRR3M (Tokai). The mean-squaredisplacement < u2 > of hydrogen atoms
was evaluated from the Q dependence ofthe elastic scattering intensity I ( Q) by using the following the Debye-Waller formula: I ( Q) = I (0) exp[-(1/3)< u2 > Q2 ],where I (0) is the elastic intensity at Q =0. In order to reduce the effect of coherent scattering, I ( Q) was devided by that at
20K.
Figure 1 shows the temperature dependence of < u2 > for the δe , γ and glass
samples. The mean square displacementof the glass sample is larger than that ofthe γ and δe phases in the whole temperature range of 100-350K. Although there isno conspicuous difference in < u2 > between the two crystalline phases, δe and γ,
up to 250K, the δe phase shows a clearlylarger displacement in the higher temperature region, which is attributable to theweaker interchain interaction in δe phase.
As for the QNS component, these samples exhibit their own characteristics; theδe phase shows a larger contribution to thehigh Qand low ΔE region, suggesting theactivation of local motions.
According to the previous 13 C-NMR
study by Gomez and Tonelli, the spinlattice relaxation times T1 are shorter inthe δe phase than the glass. We conjecture that the difference in the NMR andQNS experiments is due to the time scaleof detectable molecular motion. Considering all the various factors together, we inferthat the inﬂuence of the nonoporous structure appears most conspicuously in slow
and large motions. However, we can see
from the results of QNS that smaller molecular motions of shorter time scale, which
are probably the phenyl group’s motions,
are more activated in the nanoporous δephase. To clarify the more detailed dynamical properties of the δe phase, it is necessary to study the larger molecular motionof longer time scale.

Fig. 1. Temperature dependence of mean square displacement in sPS solid states

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 746- 204 -

JAEA-Review 2013-039

1-5-16

Static/Dynamic Structural Investigation of Lipid Nanodiscs
M. Nakano(A), M. Fukuda(A), M. Miyazaki(A), Y. Wada(A), H. Endo(B)(A)Graduate School of Pharmaceutical Sciences, Kyoto Univ., (B)ISSP-NSL, Univ. of Tokyo
Phospholipid Nanodiscs are lipid-protein
complexes in which amphipathic helices,such as apolipoprotein A-I (apoA-I) andits truncated proteins surround the edge ofthe bilayer. Nanodiscs can be formed bysimply mixing apoA-I and lipids (such as
dimyristoylphosphatidylcholine (DMPC))
at the gel-liquid crystalline phase transition
temperature of the lipid, or by solubilizing these compounds into a micellar solution of cholate with subsequent removal of
the surfactant. The reported size of Nanodiscs constituted by apoA-I ranges from 7
to 12 nm, depending on the lipid used or
lipid/protein composition. However, theirdetailed structure and characteristics, especially the dynamic properties of lipids in
Nanodiscs, are not well understood.
We previously 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]. In the present
study, we elucidated the static and dynamic properties of apoA-I/DMPC Nanodiscs with SANS.
ApoA-I was isolated from pig plasma.
DMPC was mixed with buffer containing
apoA-I (DMPC:apoA-I = 80:1 (mol/mol))and incubated at 25 °C for 8h. Nanodiscs formed were separated from coexisting vesicles and lipid-free proteins bydensity gradient ultracentrifugation. Nanodiscs consisting of either d54-DMPC (Ddisc) or DMPC (H-disc) were prepared.
SANS proﬁles of D- and H-disc with different scattering contrasts were ﬁtted simultaneously, and whole diameter was estimated at 9.4 nm. From the core volume,the molecular area of DMPC was calculated as 0.50 nm2, which is much smaller
than the molecular area in vesicles (0.66
nm2), suggesting closer lipid packing.

Time-resolved SANS measurement wasstarted immediately after mixing an equivalent volume of D-disc and H-disc. Timecourse of the normalized contrast was calculated from the scattering intensity. The
decay curves at four different temperatures were reproduced well by singleexponential function to provide the rate
constant (kex). Noteworthy, the decays
were more than 20-fold faster than the theoretical decay with the exchange rate for
LUVs. Arrhenius plot for kex suggested
that DMPC desorbs from Nanodiscs via enthalpically unfavorable but entropically favorable process. These distinct dynamic
properties of lipids in Nanodiscs, including
a decreased activation energy comparedwith LUVs, could be ascribed to the entropically more unstable state in Nanodiscs
as suggested by the static SANS measurements. That is, the lower entropy state derived from the closer lipid packing countervails the decremental entropy on the lipid
desorption.
In conclusion, the static and time-resolved
SANS study clariﬁed the fast lipid dynamics in Nanodiscs, which is connected withthe static properties of bilayers altered by
the envelopment with the proteins.
References[1] M. Nakano, M. Fukuda, T. Kudo, H.
Endo, T. Handa, Phys. Rev. Lett. 98 (2007)
238101.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-5-17

nano-meter-sized domain formation in model bio-membrane
Y. Sakuma and M. Imai
Department of Physics, Ochanomizu University
Using a contrast matching techniqueof small angle neutron scattering (SANS)
we have investigated a phase separation
to liquid-disordered and liquid-orderedphases on ternary small unilamellar
vesicles (SUVs) composed of deuteratedsaturated,hydrogenated-unsaturated
phosphatidylcholine lipids and cholesterol, where the equilibrium size of these
domains is constrained to less than 10 nm
by the system size. Below a miscibility
temperature, we observed characteristic
scattering proﬁles with a maximum, indicating formation of nano-meter-sizeddomains on the SUVs.
The observed
proﬁles can be described by a multidomain model rather than a mono-domain
model.
The nano-meter-sized domain
is agitated by thermal ﬂuctuations andeventually ruptured, which may result inthe multi-domain state. The kineticallytrapped nano-meter-sized domains growto a mono-domain state by decreasing
temperature. Furthermore, between the
miscibility and disorder-order transition
temperature of saturated lipid, the integrated SANS intensity increased slightly,
indicating the formation of nano-metersized heterogeneity prior to the domain
nucleation.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 838- 206 -

JAEA-Review 2013-039

1-5-18

Neutron Reﬂectivity Studies of the Swelling States of Polysulfobetaine Brush at
Water Interface
Y. Terayama1, M. Kobayashi １,2, A. Takahara1,2
1Institute for Materials Chemistry and Engineering, 2Graduate School of Engineering, Kyushu
University
Water-swollen states of hydrophilic polymer brushes have been paid great attention because they relate to biointerface performance and water lubrication.
We studied the swollen structure of polymer brushes containing zwitter inonic
and nonionic macromolecules in aqueous solution by neutron reﬂectivity (NR).
This article describes a part of them,focusing on swelling behavior of polysulfobetaine brush prepared by surfaceinitiated radical polymerization polymerization of (3-dimeth yl(methacryloxyethyl)ammonium propane sulfonate) (DMAPS).
Poly(DMAPS) is insoluble in pure water
due to the strong attractive electrostatic interaction between ammonium cations andsulfonyl anions. In contrast, poly(DMAPS)
is soluble in salt solution because of thescreening of the inter- or intramolecular interaction by ions in aqueous solution[1,2]. The dependence of ionic strengthon swelling behavior of poly(DMAPS)
brush was investigated by NR.
The poly(DMAPS) brush on quartz was
prepared by surface-initiated atom transfer
polymerization of DMAPS. NR was measured by a multilayer interferometer forneutrons (MINE) in JRR-3 at TOKAI, using wavelength λ = 0.88 nm with an accuracy of 2.7 %. A neutron beam was irradiated from a quartz substrate to the interface between heavy water (D2O) and thepoly(DMAPS) brush on quartz glass. The
incident slit width were adjusted to maintain a 55 mm footprint size on the sample
surface. The scattering vector, q, in specular
reﬂectivity is deﬁned by q = (4 π/λ) sin θ.
The NR proﬁles were analyzed by ﬁtting
calculated reﬂectivity from model scattering length density proﬁles to the data using
Parratt32 software.

Figure 1 shows the neutron reﬂectivity
curves and scattering length density proﬁles of poly(DMAPS) brush in D2O and
0.5 M NaCl/D2O. The neutron scattering length density (SLD) of poly(DMAPS)
brush in D2O was dramatically increased
from 4.80 × 10-4 to 6.32 × 10-4 nm-2 alongwith the distance from the substrate, andwas slightly increased up to 6.39 × 104 nm-2 at the pure D2O region. Volume
fraction distribution of DMAPS segmentsin D2O solution was evaluated from SLD
curve, and was ﬁtted by the parabolic function to estimate the brush thickness in solution, which was 130 nm in pure D2O. On
the other hand, the SLD proﬁle in 0.5 M
NaCl/D2O drastically increased to 5.50 ×
10-4 in 50 nm region from the substrate,
and gradually increase to 6.29 × 10-4 nm-2
at the external solution interface. Polymer
brush chains at the outermost region werestretched up to 260 nm from quartz surface. Hydrated salt ions screened the attractive electrostatic interaction of sulfobetainegroups to give an extended chain structure
like as an osmotically swollen brush of anelectrically neutral polymer.
References(1) Huglin M B and Radwan M A 1991
Makromol. Chem 192 2433.
(2) Kato T and Takahashi A 1996 Ber. Bunsenges. Phys. Chem. 100 784.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

Fig. 1. Figure 1. NR of PDMAPS brush in D2O
and 0.5 M NaCl/D2O solution and the corresponding ﬁts (Left). The SLD proﬁles in D2O and 0.5 M
NaCl/D2O solution to calculate the ﬁtting curves
for reﬂectivity (Right).

1-5-18- 208 -

JAEA-Review 2013-039

1-5-19Structure-Property Relationship of Particle-Polymer Mixture Solution under shear
ﬁeld
M. Shibayama, T. Matsunaga, T. Suzuki, N. Osaka, T. Nishida, H. Endo
ISSP, The University of Tokyo
The microscopic structure clay nanoparticles (Laponite XLG) and poly(ethyleneoxide)(PEO) suspension under steady
shear
has
been
investigatedbycontrast-variation small-angle neutron
scattering(CV-SANS). It is noted that theradius and thickness of the clay are 150
and 10 , respectively. The molecularweight of the PEO used is Mw = 1,000
kg/mol. The stock solution of clay and
PEO was prepared by adding PEO solution
to clay and stirring with a magnetic stirrer
until well-blended. Laponite (clay) platelet
dispersions in poly(ethylene oxide) (PEO)
aqueous solutions with various deuterious/hydrogeneous water compositions
were prepared and contrast-variation
SANS experiments were carried out.
Reversible shear-thinning behaviors wereobserved in both clay dispersions and PEO
solutions. No anisotropy was observedin SANS patterns even clay platelets arehighly anisotropic, indicating turbulent rotation of platelets by shearing. In the presence of PEO, on the other hand, the viscosity showed a hysteresis loop with strong
anisotropy (see ﬁgure). This suggests thatclay platelets are well aligned along theﬂow direction due to bridging together byoriented polymer chains.
Furthermore, by contrast-variation SANS
experiments, the following facts were disclosed. In a stationary state, a signiﬁcantnumber of PEO chains are adsorbed on theclay surface. Because of the presence of tiechains bridging neighboring clay platelets,
the viscosity is higher than that of clay dispersion without PEO chains. When the system is sheared, the adsorbed layer is destroyed and desorption occurs. However,by reducing the shear rate, polymer chains
start to adsorb on the clay platelets again.
Here, the desorption/adsorption process isvery much dependent on the history ofshearing, leading to a strong hysteresis behavior.

Fig. 1. SANS 2D-patterns for clay(3 wt%) dispersion, PEO(2 wt%) solution and clay(3 wt%)-PEO(2wt%) mixed solution

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

1-5-20Kinetic process on transition from small to large uni-lamellar vesicles
N. L. YamadaHigh Energy Accelerator Research Organization
It has been reported that the mixture ofdimyristoylphosphatidylcholine (DMPC;
14 carbons/chain) and dihexanoylphosphatidylcholine (DHPC; 6 carbons/chain)spontaneously form small uni-lamellar
vesicles (SUVs; several hundreds ofangstroms in radius) [1]. Due to high stability and monodispersity, SUVs consistingof long- and short-chain phospholipid mixtures have a potential for drug delivery,
micro reactor, as well as biomimetic system. According to experimental reports,
the SUVs are formed from small bilayeredmicelles (bicelles; approximately one
hundred angstroms in radius) above thechain melting temperature of long-chain
lipids Tc [2, 3, 4].
In this study, the transition not from bicelles but from small SUVs to large SUVs
has been found in this system. As far as
I know, this is the ﬁrst observation of the
SUV-SUV transition in aqueous solution ofamphiphilic molecules. The purpose in thisstudy is to clarify the mechanism of thistransition from the viewpoint of kinetics
by using time-resolved small angle neutron
scattering (SANS) by using SANS-U.
Figure 1(a) shows the time evolution of
SANS proﬁles after temperature jump from50◦ C to 27◦ C. The fringes due to large SUVs
gradually appeared for over ﬁve hours after cooling as shown in Fig. 1(a), while
those due to small SUVs gradually disappeared. This indicates that the size of SUVs
discontinuously changed at the SUV-SUV
transition. If small SUVs fused each otherto be large SUVs, continuous increase in
the vesicle size should be observed. Hence,
this result implies that transient bicelles
were formed during the transition.
To conﬁrm the assumption, model ﬁtting of SANS proﬁles have been performed.
Solid lines in Fig. 1(a) are the results of
the ﬁtting. Since scattering intensities areproportional to the number density of particles, the volume fractions of SUVs andbicelles can be estimated by the ﬁtting as
shown in Fig. 1(b). A minimal model describing time evolution from small to large
SUVs via transient bicelles well agrees withthe experimental results as solid lines inFig. 1(b). This indicates that the deformation from small SUVs to bicelles is the trigger for the transition to large SUVs, whichis induced by the stabilization of rim structure by decreasing temperature to near Tc .
References[1] N. E. Gabriel and M. F. Roberts, Biochemistry 23, 4011 (1984).
[2] K. M. Eum, G. Riedy, K. H. Langley, and M.
F. Roberts, Biochemistry 28, 8206 (1989).
[3] M. P. Nieh, C. J. Glinka, and S. Krueger,
Langmuir 17, 2629 (2001).
[4] N. L. Yamada, M. Hishida, and N. Torikai,
Phys. Rev. E, 79, 032902 (2009).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 892- 210 -

JAEA-Review 2013-039

1-5-21

Structural Analysis of N-isopropylacrylamide / Rod-like silica Hybrid Gels by
Contrast-variation Small-angle Neutron Scattering
Takuya Suzuki, Noboru Osaka, Hitoshi Endo, Mithuhiro Shibayama
ISSP-NSL, Univ. Tokyo,
Polymer gels, which are soft materials
that retain large amounts of solvent, canbe functionalized or strengthened by incorporation of inorganic compounds. The organic/inorganic hybrid gels thus obtained
can be of various morphologies, such as
semi-interpenetrating polymer networks
with inorganic domains as well as polymer
networks that are organically cross-linked
and then strengthened by the incorporationof inorganic compounds. In addition, there
exist organic hybrid gels free of organic
cross-links, but which are cross-linked by
the inorganic compounds via chemical or
physical cross-linking. Detailed studies on
hybrid polymer morphology, gelation dynamics, and interfacial structures between
polymers and inorganic compounds haveso far been limited by the inherent complexity of the systems. This complexity
originates from the molecular interactionsof the multi-component systems (i.e., thepolymers, the inorganic compounds, andthe solvent).
In this study, we investigated the microscopic structure of N-isopropylacrylamide(NIPAm)/rod-like silica hybrid gels. NIPAm gel is one of the widely studied thermo-responsive gels and a model
system for studying hydrophobic interactions. It is prepared by using redoxpolymerization and shows an attractive interaction with the silica surface via hydrogen bonding. It can be possible to discuss the inﬂuence of the distribution of inorganic compounds in the gel by ﬂexibly
changing not only the concentration but
also the size or the shape ( sphere or rod) of silica particles. The systematic study on
the mechanical property and microstructure of hybrid gel, which can be tuned bythese quantitative or geometrical arrangements of inorganic compounds, should beof great importance in order to design thehigh-performance gel. One of NIPAm/rodlike silica gel and three types of NIPAm/spherical silica gels, each having different silica sizes, were prepared while
maintaining an equal total volume fraction. Contrast-variation small-angle neutron scattering measurements were performed to clarify the silica shape dependence of the hybrid gel microstructure. The
presence of an adsorbed layer of NIPAm
chains on the silica surface and its dependence on silica particle size are addressed.
Fig.1 shows the intensity proﬁles for (left)
rod-like silica and (right) NIPAm/Rod-likesilica hybrid gels. In the case of rod-like silica, the distinct peak appeared in the low
Q region indicating the repulsive interaction of each particle. On the other hand,for the hybrid gels, the power law behavior
was observed due to the fractal-like aggregation of each particle. Moreover, it should
be noted that the shoulder was observedfor each sample indicating the form factorof each particle. By using these experimental data, the surface structure around silica
particles was discussed.

Fig. 1. Intensity proﬁles for Rod-like silica (left) and
NIPAm/Rod-like silica hybrid gels (right).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 908- 211 -

JAEA-Review 2013-039

1-5-22

Structural Analysis of Polyurethane Resin by Small-angle Neutron Scattering(A) Takuya Suzuki, Mitsuhiro Shibayama, (B) Kazuhiro Hatano, Masahiko Ishii(A) Institute for Solid State Physics, The University of Tokyo, (B) Paint & Finishing Design
Dept., Vehicle Material Engineering Div., TOYOTA MOTOR CORPORATION
Polyurethane resin is one of the mostfamiliar materials consisting of polyisocyanate and polyol groups. Due to thegood mechanical properties like adherence and durability, polyurethane resin is
widely used as industrial materials in thewide ranges such as adhesives, fabrics,
paints, and inks. Polyurethane resin including isocyanurate groups, which is formed
by a trimerization reaction of isocyanategroups, provides better thermal stability
and rigidity than that composed of linear
urethane bonding because of more functional groups and of stiffer hard segmentsin the former one.
As for the effect of the stoichiometric ratio, [NCO] / [OH], into the network structure of polyurethane resin, various studies
have been carried out so far. Redman reported the effect of the [NCO] / [OH] ratioon molecular weight and on the rheological, thermal, and mechanical properties of
two series of ester-based polyurethanes.[1]Nierzwicki and Wysocka also studied theeffect of the [NCO] / [OH] ratio on
the micro-phase separation of ester-based
polyurethanes, which can be induced by
the soft segments and hard segments, bythermo-mechanical analysis (TMA).[2]In this paper, we discuss the gelation kinetics and the microstructure of polyurethanegels by focusing on the network concentration and the stoichiometric ratio of isocyanate to hydroxyl groups, [NCO] / [OH].
The purpose of this study is to clarify thefollowing matters, i.e., the effect of the total concentration and [NCO] / [OH] on
the microscopic inhomogeneities of the network. We used acryl-polyol as a soft segment component and polyisocyanate as a
hard segment component.
Fig.1 shows the intensity proﬁles ofpolyurethane resin having different total

concentration(wt%) and [NCO] / [OH]. In
the case of 12.8 wt%, the [NCO] / [OH]dependence is so little and the intensity
is low. This is due to the fact that at 12.8
wt%, the system was at liquid state while
the sample became gel-like state by further increasing the total concentration. Itshould be noted that at 17.1 wt%, the intensity became the maximum. At more than
17.1 wt%, the intensity decreased with thetotal concentration due to the decrease of
the concentration ﬂuctuation of the polymer network. These experimental results
were also in good agreement with our previous work by dynamic light scattering.[3]At 54 wt%, the intensity proﬁles were ﬂatdue to the strong incoherent scattering of
the concentrated polymers.
References[1]Redman
RP.
DevelopmentsinPolyurethanes. London: Applied Science
Publishers, 1978.
[2]Nierzwicki W and Wysocka E. J. App.
Polym. Sci. 1980;25:739-746.
[3]T. Suzuki, M. Shibayama, K. Hatano, and
M. Ishii. Polymer, in press.

Fig. 1. Intensity proﬁles of polyurethane resin.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 911- 212 -

JAEA-Review 2013-039

1-5-23

Small-angle neutron scattering study of block copolymers in supercritical carbon
dioxideM. Itoh, H. Yokoyama, K. Mayumi, K. Ito, N. Osaka, H. Endo, M. Shibayama
University of Tokyo
Depending on volume fraction of eachblock, degree of polymerization and interaction between blocks, several microphaseseparated morphologies are observed indiblock copolymers. These morphologies
are kinds of micro-phase separation ofeach blocks: Examples are spheres, cylinders and lamellae ordering in long-ranged
periodic structures, such as cubic latticeof spheres and hexagonal lattice of cylinders. In addition to those classic morphologies, 3D contineous networking structures,
which are called bicontinuous structures,
have been reported. We have succeeded
in inducing multiple order-to-order phasetransitions by swelling selectively CO2philic blocks with supercritical CO2 andchanging pseudo-volume fraction. Thismorphology change was anticipated by exsitu analysis of the samples frozen and removed from supercritical CO2. However,in-situ measurement of selectively swollen
block copolymers in supercritical CO2 has
never been conducted. Thus this time we
performed in-situ measurement of swollen
block copolymers in CO2 by neutron scattering analysis.
We analyzed the morphologies ofPoly(styrene-b-perﬂuorooctylethyl
methacrylate)s (PS-PFMAs), using small
angle neutron scattering measurement
system ,SANS-U, at JRR-3. PFMA is CO2philic and highly swollen in CO2. We
prepared three samples differing withthe ratio of PS to PFMA and total degreeof polymerization, of which molecularweights and weight fraction of PFMA are
18,600 and 20 % (S1), 17,400 and 48% (S2),and 23,000 and 28 wt% (L), respectively.
Samples for SANS were made by castingfrom triﬂuorotoluene solutions. Then thesamples were placed into high-pressure
cell with CO2 pressure and temperature

controls. This time, temperature was ﬁxed
at 60 degree C and pressure was varied
from atmospheric pressure to 30MPa.
Fig.1 shows the pressure dependence of
SANS proﬁles. Proﬁles in each graph areseriated in increasing order of pressure.
Fig1a is scattering patterns of S1. At 0.1MPa
the peak positions of q (1:1.73), corresponding to Hex lattice of PFMA Cylinders
is found. Similarly, the proﬁle at 15MPa
agrees with lamellar peak pattern. At 10
MPa, at which the effective volume fraction is between cylinderical and lamellar
morphologies, unknown peak pattern appeared. Because the ﬁrst and second order peaks were not well separated due tolimited resolution, we cannot assign themorphologies at this point, but the peakratio is inconsistent with either cylinder
or lamellar. Pressurizing from 15MPa to
20MPa we observed sudden change of theﬁrst peak position followed by BCC/SC
lattice of spheres at 25MPa and 30MPa(1:1.44). The sudden change of the ﬁrst order peak position can be interpreted as evidence of exchange of the matrix. Scattering
proﬁles of S2 with higher PFMA fraction(48%) is shown in Fig.1b. In as cast state,peaks appear at 1, 1.99, 2.97 relative to theﬁrst order, which is lamella. In pressurizing process at 15 MPa, peak ratio 1:1.74:1.86
was observed. This pressure and hence theeffective volume fraction is in bicontinuous regime, but identifying this structure
requires additional experiments. As pressurizing continuously, the polymer structure changed to Hex of cylinder at 25MPa
and ﬁnally the structure factor vanished at
30MPa.
Fig.1c shows the scattering function of Lwith the higher mass. From peak ratios ofas cast specimen and at the pressure upto
20MPa, the morphology is always Lamella.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 917- 213 -

JAEA-Review 2013-039

At a pressure over 25MPa peak becomes
weak, and at 30MPa structure factor completely disappears.
As can be seen from these three samples,
we observed multiple order-to-order transitions. We are continuing in-situ measurement with SANS on new additional samples with different ratio of PFMA and thedegree of polymerization.

Fig. 1. Fig. 1. Small angle neutron scattering patterns of PS-PFMAs with different molecular weight
and fractions at several different CO2 pressures: (a)Mn = 18,600 and PFMA wt% = 20; (b) 17,400 and48%; (c) Mn = 23,000 and PFMA = 28 wt%.

1-5-23- 214 -

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1-5-24

Reconstruction of uni-lamellar vesicles induced by addition of polymers
N. L. YamadaHigh Energy Accelerator Research Organization
tional to the size of SUVs. The size of
SUVs after the addition of PEG solution depends on the molecular weight of the PEG.
However, the origin of the reconstructionof SUVs has not been understood yet.
References[1] N. E. Gabriel and M. F. Roberts, Biochemistry 23, 4011 (1984).
[2] N. L. Yamada, M. Hishida, and N. Torikai,
Phys. Rev. E, 79, 032902 (2009).
[3] S. Okabe, M. Nagao, T. Karino, S. Watanabe, T. Adachi, H. Shimizu, and M.
Shibayama, J. Appl. Cryst. 38, 1035 (2005).
6

10

5

10

4

10
I(q) [arb. unit]

It has been reported that the mixtureof long-chain phospholipids (14 carbons/chain or more) and short-chain
phospholipids (6 − 8 carbons/chain) spontaneously forms small uni-lamellar vesicles(SUVs; several hundreds of angstroms inradius) [1]. Since a membrane consistingof phospholipid molecules is the main
component of biomembranes, such SUVs
have a potential to create biomimetic
system for studying bioactivities incells. Recently, it has been reported that
nanopores are sponetaneously formedon the surface of SUVs consisting of
dimyristoylphosphatidylcholine (DMPC;
14 carbons/chain) and dihexanoylphosphatidylcholine (DHPC; 6 carbons/chain)mixture [2]. If translocation of polymers
thorough the nanpores can be observed,
this system would be an ideal system toinvestigate the material transportation inreal cells.
In this study, the effect of polyethyleneglycol (PEG) on the stability of SUVs consisting of DMPC and DHPC mixture has been
investigated by small angle neutron scattering (SANS) for the ﬁrst step. The SANS
experiments were performed using SANSU at the C1-2 port of JRR-3 at Japan Atomic
Energy Agency (JAEA), Tokai [3]. The lipid
mixture of [DHPC]:[DMPC] = 1:3.2 was
dissolved in a D2 O solution of 3 mM CaCl2 .
The lipid concentration of the solution was
controlled to be 0.9 vol%. The obtained solution was kept at 30◦ C for thirty minutes
to make homogeneous SUV solution, andmixed with the twice amount of PEG solution (100 mg/mL PEG and 3 mM CaCl2 ).
Figure 1 shows the SANS proﬁles after
the addition of PEG solution. The periodof fringes becomes shorter than that before
the addition. This result indicates that thereconstruction of SUVs occured, because
the period of fringes is inversely propor-

3

10+PEG: 40k

2

10

1

10

+PEG: 4k

before PEG addition

0

10

-1

10

-2

10
2
0.001

4

6 8

2

0.01
-1
q [Å ]

4

6 8

0.1

2

4

Fig. 1. SANS proﬁles before and after the additionof PEG solution.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 925- 215 -

JAEA-Review 2013-039

1-5-25

Relation between bending modulus and spontaneous curveture in DGI/SDS/D2O
system
H. Mayama(A), X. J. Chen(A), M. Nagao(B), H. Seto(C) and K. Tsujii(A)(A)Nanotechnology Research Center, RIES, Hokkaido Univ., (B)ISSP-NSL Univ. Tokyo,(C)Dept. Phys, Kyoto Univ.
A non-ionic surfactant, n-dodecyl glyceryl
itaconate (DGI), self-assembles into bilayer
membranes in water having a spacing distance of sub-micrometer in the presenceof small amounts of ionic surfactants, andforms multi-lamellar structure which indicates beautiful iridescent color becauseof Bragg diffraction. We have found thatthe repeat distance between the bilayers
distributes in the scale range between 130
nm (red) and 180 nm (blue) in the suitable concentration range of ionic surfactant and it decreases with increasing theconcentration (J. Colloid Inf. Sci. 305 (2007)308). In order to understand fundamental
question why this system maintains long
repeat distance on the order of 100 nm,
we have studied on membrane dynamics
in the DGI/SDS/D2O system. We foundthat the membrane dynamics can be described very well by the theory of Zilman
and Granek (PRL 77 (1996) 4788) and bending modulus kappa was increased from 20
kT to 40 kT with increasing the concentration of SDS (decreasing of repeat distance) as shown in Fig. 1. Through otherexperiments on direct observation of multilamellar structure in our previous study,
we found that self-assembled DGI forms
giant onions consisted of the stacked DGIbilayers and the radius of curvature ischanged between 10 (higher SDS concentration, onion structure) and several hundred micrometer (lower SDS concentration,
ﬂat onion structure). The relation between
the spontaneous curvature and the bending modulus would give us a clue to understand the question.

Fig. 1. Iridescent color of DGI/SDS/D2O system(a) and dependence of bending modulus kappa on
SDS concentration. The insets: schematic representation of onion structures consisted of stacked layers
at lower (left) and higher SDS concentrations (right).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 931- 216 -

JAEA-Review 2013-039

1-5-26

Conformation and Dynamics of Polyrotaxane in Solution
Koichi Mayumi, Hitoshi Endo, Noboru Osaka, Hideaki Yokoyama, Mitsuhiro
Shibayama, Kohzo Ito
Graduate School of Frontier Sciences, The University of Tokyo, Institute for Solid State Physics,
The University of Tokyo
Polyrotaxane
(PR)
is
a
typicalsupramolecule, in which cyclic molecules
are threaded onto a linear polymer chain[1]. The cyclic molecules in PR can slide
and rotate on the polymer chain, and thedegree of freedom of movement within achain is the most unique feature of PR. Thisadditional kinetic freedom has been utilized to produce functional nanomaterials
having novel dynamical properties [2]. For
example, PR, composed of polyethylene
glycol (PEG) and α-cyclodextrins (CDs),
was applied to a novel kind of polymer
network, called slide-ring gel [3], which
was prepared by cross-linking CDs belonging to different PR. The cross-linking
point of slide-ring gels can slide along thepolymer chain, and this unique structurecauses the high extensibility and huge
degree of swelling ratio in slide-ring gels.
These remarkable physical properties were
derived from nanoscale sliding motion of
cyclic molecules.
We investigated the conformation and dynamics of polyrotaxane (PR) composedof polyethylene glycol (PEG) and αcyclodextrins (CDs) by means of small angle neutron scattering (SANS) and neutron
spin echo (NSE) technique, respectively.
We analyzed the scattering functions forpolyrotaxane in DMSO using a form factor
based on the wormlike chain model, and it
was found that the persistence length for
PR dissolved in DMSO was approximately
30 , which is three times as large as thatof PEG dissolved in DMSO [4]. Furthermore, the monomer dynamics of PR observed by NSE measurements was slower
than that of PEG [5]. These ﬁndings indicate that threading CDs into PEG stretched
the PEG chain and suppressed the local dynamics.

[1] A. Harada, J. Li, M. Kamachi, Nature(London) 356, 325 (1992)..
[2] J. Araki, K. Ito, Soft matter 3, 1456
(2007).
[3] Y. Okumura, and K. Ito, Adv. Mater. 13,
485 (2001).
[4] K. Mayumi, N. Osaka, H. Endo, H.
Yokoyama, Y. Sakai, M. Shibayama, K. Ito,
Macromolecules, 41, 6480 (2008).
[5] K. Mayumi, N. Nagao, H. Endo, N. Osaka, M. Shibayama, K. Ito, Physica B, inpress.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 946- 217 -

JAEA-Review 2013-039

1-5-27

Mechanically Interlocked Structure of Polyrotaxane Investigated by Contrast
Variation Small Angle Neutron Scattering
Koichi Mayumi, Hitoshi Endo, Noboru Osaka, Hideaki Yokoyama, Mitsuhiro
Shibayama, Kohzo Ito
Graduate School of Frontier Sciences, The University of Tokyo, Institute for Solid State Physics,
The University of Tokyo
Advances of supramolecular chemistry hasrealized novel polymer architectures composed of several components noncovalently bonded [1]. One of the most promising supramolecules is polyrotaxane (PR) in
which cyclic molecules are threaded into aliner polymer chain [2]. Covering the axial
polymer chain with the cyclic molecules resulted in various applications to nanomaterials such as molecular tubes formed bycross-linking adjacent cyclic molecules in asingle polyrotaxane and insulated molecular wires incorporating conductive polymers. The cyclic molecules in polyrotaxane
are mechanically interlocked with the axial
polymer, and slide and rotate on the chain.
This additional kinetic freedom has beenutilized to produce functional nanomaterials having novel dynamical properties, examples of which are drug delivery systems,
multivalent ligand systems, energy transfer systems, and three-dimensionally crosslinked polyrotaxane networks with movable crosslinks. In particular the mechanically interlocked structure of polyrotaxane
leads to various application to nanomaterials.
We performed contrast variation small angle neutron scattering measurements onpolyrotaxane composed of polyethylene
glycol (PEG) and α-cyclodextrins (CDs) inorder to determine the detailed structureof PEG and CD in polyrotaxane. The scattering intensities I(Q) s for PR in mixtures of DMSO-d6 and DMSO were successfully decomposed into partial scattering functions for the components of polyrotaxane. The CD-PEG cross-term is positive, which corresponds to the mechainically interlocked connection between PEG
and CD. In addition, the self-term of CD

showed almost the same Q-dependence as
the self-term of PEG. This indicated that theCDs in polyrotaxane are distributed randomly along the PEG chain. Contrast variation SANS is efﬁcient to investigate static
structures of components in supramolecular systems such as the conformations ofand the correlations between the components in the system.
[1] Lehn, J. M. Supramolecular Chemistry:
Concepts and Perspectives, VCH, Weinheim, 1995.
[2] Harada, A.; Hashidzume, A.;
Takashima, Y. Adv. Polym. Sci. 2006,
201, 1.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 947- 218 -

JAEA-Review 2013-039

1-5-28QENS Study on Thermal Gelation in Agarose Aqueous Solution
N. Onoda-Yamamuro(A) and O. Yamamuro(B)(A) Tokyo Denki Univ., (B) ISSP-NSL, Univ. Tokyo
Thermoreversible gelation of aqueous
solution of macromolecules is due to theformation of a physically crosslinked network structure. Macroscopic properties,
such as viscosity, change drastically withgelation. It is of interest whether microscopic motions such as diffusion of water molecules and segmental vibration ofmacromolecular chains change or not withgelation. Methylcellulose (MC) gels onheating due to hydrophobic interactions
between methoxyl groups. We have shownthat dynamic slowing down occurs not
only for macroscopic properties but also for
microscopic motion of both MC and water molecules by quasi-elastic neutron scattering (QENS) measurements [1]. In thisstudy thermal gelation of agarose was examined. Agarose (AG) gels on cooling due
to formation of hydrogen bonds.
QENS experiments were performed on
AG solution using AGNES spectrometer,
installed at C3-1 port of JRR-3M in Tokai.
D2O, not H2O, was used as a solvent toobserve both dynamics of water and AG
molecules. The relative scattering intensityfrom H atoms of agarose to that from D
atoms of D2O is expected to be comparable in this sample solution. The sample (3.0
wt-% solution) in this study geled around
315K on cooling and soled around 370K on
heating.
The data were ﬁtted well to the sum ofa Lorentzian function and a Delta function,
both of which are convoluted by resolutionfunction as shown in Fig. 1 (a). The former is attributed to diffusive motion of water molecules and the latter to local vibrational motion of AG molecules. The selfdiffusion coefﬁcient D of water molecules
was obtained from the Q-dependence ofthe HWHM of the Lorentzian function,
while the mean square displacement u2 of
AG molecules was obtained from the Q-

dependence of the intensity of the Delta
term. Temperature dependence of D and
u2 are shown in Fig.1 (b). The meansquare displacement abruptly decreased
and the slope of the self-diffusion coefﬁcient changed with gelation on cooling.
The present results revealed that the microscopic motions of both water and AG
molecules give rise to dynamic slowing
down on thermal gelation.
[1] N. Onoda-Yamamuro et al. Physica B
Condens. Matter, 393, 158 (2007).

Fig. 1. Figure 1(a) An example of ﬁts to S(Q,E) of the
AG solution. (b) T dependence of the self-diffusion
coefﬁcient D of water and the mean square displacement <u2> of the local motion in AG molecules.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 960- 219 -

JAEA-Review 2013-039

1-5-29Aggregation Structure and Dynamics of Polymers at the Interface with Water I:
Analysis of Aggregation Structure by Neutron Reﬂectivity
Hironori Atarashi(1), Toshihiko Nagamura(1), Masahiro Hino(2), Keiji Tanaka(1)1.Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2.
Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
Recently, a microwave treatment has been
widely adopted for polymer synthesis because the treatment accelerates the movement of reactants in the system. The advantage of the treatment is not only shortening of the reaction time but also easy controlling of the yield and tacticity. However, it seems to us that the effectiveness ofthe microwave treatment on time evolutionof aggregation states in polymer solids has
not been discussed yet. In this study, we
examined the microwave effect on interfacial evolution of polystyrene (dPS) bilayerswith the aid of neutron reﬂectivity (NR) so
that acceleration of chain diffusion by microwave can be discussed.
Monodisperse PS and deuterated PS (dPS)
were used as samples. Molecular weights
of PS and dPS were 87k and 80k, respectively. A dPS ﬁlm was prepared on a silicon (Si) substrate with a native oxide layer
by a spin-coating method. And, a PS ﬁlm,
which was independently spin-coated ona glass substrate, was mounted onto thedPS ﬁlm by a ﬂoating method. Each ﬁlm
thickness was approximately 50 nm. The
PS/dPS ﬁlms so-prepared were dried under vacuum for 24 h at room temperature,and microwave with the power of 150 W
was irradiated on them under the ambient
atmosphere for 1.5 min and 3 min. Then,the specimens were applied to NR measurements using MINE2 spectrometer.
Figure 1 (a) shows the NR proﬁles for the
PS/dPS bilayer ﬁlms before and after the
microwave treatment. The open symbols
denote experimental data and solid lines
show bets-ﬁtting curves calculated on thebasis of the model scattering length density (b/V) proﬁles shown in the panel (b)of Figure 1. The interface between PS anddPS layers before the treatment was sharp.

The width is basically arisen from the surface roughness of the original PS and/or
dPS ﬁlm/s. On the other hand, once thebilayer was treated by microwave, the interface disappeared and the (b/V) value
in the internal region became 3.72 x 104 nm-2, which was almost the middle ofthe (b/V) values for PS and dPS. Thismeans that PS and dPS chains interdiffusedeach other, resulting in the formation of homogenous phase in the ﬁlm. The (b/V)
proﬁles treated for 1.5 min and 3 min were
almost the same. Thus, chain interdiffusionin the bilayer reached a quasi-equilibrium
state even by the 1.5 min.-treatment. Interestingly, the (b/V) value was higher near
the substrate interface than in the interior region. This makes it clear that thedPS component was enriched at the substrate interface in the ﬁlm being in a quasiequilibrium state. The detail mechanism of
how the treatment affects on chain diffusion, especially, a thermal effect induced bysurrounding substance, will be reported in
the near future.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 972- 220 -

JAEA-Review 2013-039

Fig. 1. Figure 1 (a) Neutron reﬂectivity for a PS/dPS
ﬁlm treated by microwave for 0, 1.5, and 3 min. The
scattering length density proﬁles is shown in (b).
For clarify, each data is off-set by a decade.

1-5-29- 221 -

JAEA-Review 2013-039

1-5-30Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: II. Analysis of Relaxation Dynamics by Neutron Spin Echo
Hironori Atarashi(1), Toshihiko Nagamura(1), Keiji Tanaka(1), Hitoshi Endo(2), andMitsuhiro Shibayama(2)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2. Institutefor Solid State Physics, The University of Tokyo, Chiba 277-8581, Japan
Recently, polymer and liquid interface is widely studied, because aggregation
states of polymers at liquid interface areimportant for science and technological application such as lubricate, adhesive, andbiocompatibility. We have studied about
the structure of poly(methyl methacrylate)(PMMA) contacted with non-solvent byusing neutron reﬂectivity and scanning
force microscope.[1] As a result, waterand methanol, in spite of non-solvent for
PMMA, made PMMA ﬁlm swollen. In
this study, the swollen structure, especiallythe interface structure between PMMA andnon-solvent, of PMMA particles were studied by using small angle neutron scattering
instrument, University of Tokyo (SANS-U)
and new issp neutron spin echo (iNSE).
PMMA particles with diameter of about300-500 nm (MP-2200 produced by Soken
Chemical & Engineering Co., Ltd.) wereused as a sample. Deuterated water (D2O)
and deuterated methanol (CD3OD) wasused as a non-solvent. The PMMA particles mixed with non-solvent were ﬁlled
into quartz cell with 2 mm optical length.
The sample-to-detector distance was chosen to be 2 and 12 m.
Figure 1 (a) shows the SANS proﬁles for PMMA particles on 25 and 40 °C mixed with water. Incoherent component was bated as background, and the proﬁles were ﬁtted with power function. The
value of ﬁtted power was almost about 4
both in whole q region. It means that theshape of PMMA particles was not changed
with temperature change. Additionally, tosee more detail in small range, Porod plot
was carried on. As a result, the power forq increased with increasing temperature.
It means that the interfacial thickness be-

tween PMMA and water became broader
with temperature increasing. Figure 1(b)shows the SANS proﬁles for PMMA particle mixed with methanol. In high q region,
it is clear that the value of power was lower
than it in low q region. That means theinterfacial thickness between PMMA andmethanol is broad and that broadening isbigger in compared with the case of water. We performed iNSE measurement using same sample. A certain relaxation wasobserved in the case of PMMA particles in
D2O at 85 °C. We will clarify the dynamics of PMMA chain at the interface between
PMMA and non-solvent.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 978- 222 -

JAEA-Review 2013-039

1-5-31

An Eﬀect of Electromagnetic Wave Treatment on Polymer Diﬀusion
Hironori Atarashi(1), Toshihiko Nagamura(1), Masahiro Hino(2), Keiji Tanaka(1)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2. Resarch
Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
Recently, a microwave treatment has been
widely adopted for polymer synthesis because the treatment accelerates the movement of reactants in the system. The advantage of the treatment is not only shortening of the reaction time but also easy controlling of the yield and tacticity. However, it seems to us that the effectiveness ofthe microwave treatment on time evolutionof aggregation states in polymer solids has
not been discussed yet. In this study, we
examined the microwave effect on interfacial evolution of polystyrene (dPS) bilayerswith the aid of neutron reﬂectivity (NR) so
that acceleration of chain diffusion by microwave can be discussed.
Monodisperse PS and deuterated PS (dPS)
were used as samples. Molecular weights
of PS and dPS were 87k and 80k, respectively. A dPS ﬁlm was prepared on a silicon (Si) substrate with a native oxide layer
by a spin-coating method. And, a PS ﬁlm,
which was independently spin-coated ona glass substrate, was mounted onto thedPS ﬁlm by a ﬂoating method. Each ﬁlm
thickness was approximately 50 nm. The
PS/dPS ﬁlms so-prepared were dried under vacuum for 24 h at room temperature,and microwave with the power of 150 W
was irradiated on them under the ambient
atmosphere for 1.5 min and 3 min. Then,the specimens were applied to NR measurements using MINE2 spectrometer.
Figure 1 (a) shows the NR proﬁles for the
PS/dPS bilayer ﬁlms before and after the
microwave treatment. The open symbols
denote experimental data and solid lines
show bets-ﬁtting curves calculated on thebasis of the model scattering length density (b/V) proﬁles shown in the panel (b)of Figure 1. The interface between PS anddPS layers before the treatment was sharp.
The width is basically arisen from the sur-face roughness of the original PS and/or
dPS ﬁlm/s. On the other hand, once thebilayer was treated by microwave, the interface disappeared and the (b/V) value
in the internal region became 3.72 x 104 nm-2, which was almost the middle ofthe (b/V) values for PS and dPS. Thismeans that PS and dPS chains interdiffusedeach other, resulting in the formation of homogenous phase in the ﬁlm. The (b/V)
proﬁles treated for 1.5 min and 3 min were
almost the same. Thus, chain interdiffusionin the bilayer reached a quasi-equilibrium
state even by the 1.5 min.-treatment. Interestingly, the (b/V) value was higher near
the substrate interface than in the interior region. This makes it clear that thedPS component was enriched at the substrate interface in the ﬁlm being in a quasiequilibrium state. The detail mechanism of
how the treatment affects on chain diffusion, especially, a thermal effect induced bysurrounding substance, will be reported in
the near future.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 979- 223 -

JAEA-Review 2013-039

Fig. 1. Figure 1 (a) Neutron reﬂectivity for a PS/dPS
ﬁlm treated by microwave for 0, 1.5, and 3 min. The
scattering length density proﬁles shown in (b). For
clarify, each data is off-set by a decade.

1-5-31- 224 -

JAEA-Review 2013-039

1-5-32Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: I. Analysis of Aggregation Structure by Neutron Reﬂectivity
Hironori Atarashi(1), Toshihiko Nagamura(1), Masahiro Hino(2), Keiji Tanaka(1)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2.
Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
When a polymer material is used asa biomaterial in human body, the polymer surface is contact with liquid such as
blood. Thus, to know the detail of interface between polymer and liquid is important to make high functional materials. In
this study, we evaluated the swollen structure of poly(methyl methacrylate) (PMMA)
contacted with alcohols.
A deuterated PMMA (dPMMA) withmolecular weight of 296k was used as asample. A dPMMA ﬁlm was spin-coatedonto quartz from dPMMA toluene solution. The ﬁlm thickness was adjusted toabout 65 nm. The ﬁlm was annealed for
24 h at 423 K under vacuum. Ethanol,
1-propanol, and 2-propanol were used as
non-solvent.
Figure 1 (a) shows the NR proﬁlesfor the dPMMA ﬁlms under air, ethanol, 1propanol, and 2-propanol. The open symbols denote experimental data and solidlines show bets-ﬁtting curves calculated on
the basis of the model scattering lengthdensity (b/V) proﬁles shown in the panel(b) of Figure 1 (Figure 1 (b) was normalized with initial thickness in air). The dPMMA ﬁlms were swollen under all alcohols. However, the swollen behavior wasdifferent by alcohol. In the case of ethanol,
ethanol diffused into dPMMA ﬁlm andthe ethanol contents in whole ﬁlm was 13
vol.%. Then ﬁlm thickness of dPMMA contacted with ethanol increased and the ration of increasing ﬁlm thickness was 1.19,
and the interface between dPMMA andethanol became rough. Also, in the case ofboth 1-propanol and 2-propanol, dPMMA
ﬁlms were swollen and alcohol contents
was 5.7 vol.%. Then the ﬁlm thickness ofdPMMA in contact with both 1-propanoland 2-propanol increased and the ratio was

1.12. Interestingly, all alcohols through thedPMMA ﬁlm and segregated to quartz interface. The detail of swollen structure andswollen mechanism of dPMMA under alcohols will be reported in the near future.

Fig. 1. Figure 1 (a) Neutron reﬂectivity for a dPMMA ﬁlms under air, ethanol, 1-propanol, and 2propanol. The scattering length density proﬁles isshown in (b). For clarify, each data is off-set by adecade.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 980- 225 -

JAEA-Review 2013-039

1-5-33Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: I. Analysis of Aggregation Structure by Neutron Reﬂectivity
Hironori Atarashi(1), Toshihiko Nagamura(1), Masahiro Hino(2), Keiji Tanaka(1)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2.
Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
New tools for tailor-made diagnostics are
generally made from polymers. In theseapplications, the polymer surface is in contact with a water phase. However, despite the importance of detailed knowledgeof the fundamental interactions of polymer interfaces with liquids, such studies
are very limited. We have hitherto studied aggregation structure of poly(methyl
methacrylate) (PMMA) at the interfaces
with non-solvents such as water, hexane and methanol by neutron reﬂectivity.[1] As a result, the liquid/polymer interfaces were diffuse in comparison withthe air/polymer interface, probably due tointerfacial roughening and the partial dissolution of segments at the outermost region of the ﬁlm. In this study, we focus
on alcohol with different alkyl lengths as
non-solvents so that an impact of solubility parameter on the interfacial aggregation states can be discussed. A deuterated
PMMA (dPMMA) with number-averagemolecular weight of 296k was used as asample. A ﬁlm of dPMMA was spincoated onto a quartz block from a toluene
solution. The ﬁlm thickness was adjusted
to be about 65 nm. The ﬁlm was annealedfor 24 h at 423 K under vacuum. Ethanol,
1-propanol, and 2-propanol were used as
non-solvents.
Figure 1 (a) shows the NR proﬁlesfor the dPMMA ﬁlms under air, ethanol, 1propanol, and 2-propanol. The open symbols denote experimental data and solidlines show best-ﬁtting curves calculated on
the basis of the model scattering lengthdensity (b/V) proﬁles shown in the panel(b), where the abscissa was normalizedwith the initial thickness in air. While thedPMMA ﬁlm was discernibly swollen under all alcohols, the extent was not the sameamong them. Interestingly, the segregationof alcohol molecules was observed at thesubstrate interface for all the cases. The
overall contents of ethanol, 1-propanol and2-propanol in the ﬁlm were 13, 5.7 and 5.7
vol.%, respectively. The solubility parameters for ethanol, 1-propanol, 2-propanoland PMMA are, respectively, 26.0, 24.3, 23.5
and 22.7. Thus, to what extent alcohol
molecules penetrate into the ﬁlm can be
hardly explained only in terms of the solubility parameter. The size of penetrants
should be also taken into account.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 984- 226 -

JAEA-Review 2013-039

1-5-34Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: II. Analysis of Relaxation Dynamics by Neutron Spin Echo
Hironori Atarashi(1), Toshihiko Nagamura(1), Keiji Tanaka(1), Hitoshi Endo(2), andMitsuhiro Shibayama(2)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2. Institutefor Solid State Physics, The University of Tokyo, Chiba 277-8581, Japan
New tools for tailor-made diagnostics are
generally made from polymers. In theseapplications, the polymer surface is in contact with a water phase. However, despite the importance of detailed knowledgeof the fundamental interactions of polymer interfaces with liquids, such studies
are very limited. We have hitherto studied aggregation structure of poly(methyl
methacrylate) (PMMA) at the interfaces
with non-solvents by neutron reﬂectivity.[1] As a result, the liquid/polymer interfaces were diffuse in comparison withthe air/polymer interface, probably due tointerfacial roughening and the partial dissolution of segments at the outermost region of the ﬁlm. In this study, relaxation
dynamics of PMMA chains at the interfaces
with typical non-solvents such as waterand methanol was discussed on the basisof small angle neutron scattering (SANSU) and neutron spin echo (iNSE) measurements. PMMA particles with diameter ofabout 300-500 nm (MP-2200 produced by
Soken Chemical & Engineering Co., Ltd.)
were used as a sample to increase the scattering volume rather than a ﬁlm. Deuterated water (D2O) and ethanol (CD3OD)
were used as non-solvents. The PMMA
particles mixed with a non-solvent were
ﬁlled into a quartz cell with 2 mm optical length. The sample-to-detector distancewas chosen to be 2 and 12 m.
Figure 1 (a) shows the SANS proﬁlesfor PMMA particles with water, which theincoherent contribution was subtracted, at
25 and 40 °C. The power for the linear relation was approximately 4 for bothcases. Taking into account that the specimen was PMMA particles, the result isquite reasonable. Interestingly, the power

seems to deviate from 4 at q>10-1 A-1 at 40°C. This may indicate that the interface between PMMA and water became broader
with increasing temperature. Figure 1(b)shows the SANS proﬁles for PMMA particles with methanol. In this case, the slope
transformed 4 to smaller once q went beyond 5*10-2 A-1. This means that the interface between PMMA and methanol wasquite diffused in comparison with the caseof water. Then, iNSE measurement wasmade using the same sample. A certain
relaxation was somehow observed both in
the case of PMMA particles with D2O and
CD3OD. The detail analysis for the results
has undergone several revisions.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 985- 227 -

JAEA-Review 2013-039

Fig. 1. Figure 1 Temperature dependence of SANS
proﬁles (a) in D2O and (b) in CD3OD.

1-5-34- 228 -

JAEA-Review 2013-039

1-5-35Large scale structure and crossover of critical phenomena induced by solvationeﬀect
Seto H., Sadakane K. 1 , Iguchi N.1 , and Endo H.2
Institute of Materials Research Science, KEK, 1 Department of Physics, Kyoto Univ., 2 ISSP,
Univ. of Tokyo
The binary mixture of water and 3methylpyridine, which shows LCST typephase separation, is known to have alarge salt effect. In this study, we selected sodium tetraphenylborate (NaBPh4 ),whose afﬁnities of anion and cation withwater are largely different, as a salt because
the solvation effect should be intensive andthe formation of large clusters is expected
theoretically. In cases of the lower amountof NaBPh4 and water-rich concentration,
the mixture becomes colored in blue, andchanges to orange with approaching critical temperature. This result suggests that aperiodic structure is formed, and its repeat
distance increases with increasing temperature. For the mixtures with 100 mM
NaBPh4 , the SANS proﬁles have a peakaround Q =0.1 A−1 , and the peak position
shifts to lower-Q with increasing temperature. (K. Sadakane et al., J. Phys. Soc. Jpn.
76, 113602 (2007).)
In order to investigate the solvation effect by adding NaBPh4 , further experiments are performed at SANS-U. The scattering proﬁles are successfuly interpretedwith the function proposed by Onuki and
Kitamura. The temperature dependence ofthe critical concentration ﬂuctuation shows
3D-Ising behavior when the salt concentration is low enough. On the other hand,the critical behavior is changed to 2D-Isingwith increasing the salt concentration. This
result can be interpreted that the concentration ﬂuctuation is limited in 2 dimensional
region due to the emergence of the layered
structure. This crossover is reproduced in
the cases of adding ionic surfactant suchas AOT and SDS. Thus we conclude thata membrane-like structure is formed near
the critical point by the coupling of the sal-vation effect and the critical concentration
ﬂuctuation as suggested by Onuki and Kitamura theoretically.
Neutron Spin Echo experiments are performed at iNSE in the mixture of water, 3MP and NaBPh4 . The intermediated correlation function can be interpretedwith the model proposed by Zilman andGranek. This evidence veriﬁes the formation of the membrane-like structure byadding NaBPh4 .

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 1003

- 229 -

JAEA-Review 2013-039

1-5-36Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: I. Analysis of Aggregation Structure by Neutron Reﬂectivity
Hironori Atarashi(1), Toshihiko Nagamura(1), Masahiro Hino(2), Keiji Tanaka(1)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2.
Research Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
New tools for tailor-made diagnostics are generally made from polymers.
In these applications, the polymer surface
is in contact with a water phase. However, despite the importance of detailed
knowledge of the fundamental interactions of polymer interfaces with liquids,
such studies are very limited. We have
hitherto studied aggregation structure ofpoly(methyl methacrylate) (PMMA) at theinterfaces with non-solvents such as water,
hexane and methanol by neutron reﬂectivity.[1] As a result, the liquid/polymer interfaces were diffuse in comparison withthe air/polymer interface, probably due tointerfacial roughening and the partial dissolution of segments at the outermost region of the ﬁlm. In this study, we focus
on alcohol with different alkyl lengths as
non-solvents so that an impact of solubility parameter on the interfacial aggregation states can be discussed. A deuterated
PMMA (dPMMA) with number-averagemolecular weight of 296k was used as asample. A ﬁlm of dPMMA was spincoated onto a quartz block from a toluene
solution. The ﬁlm thickness was adjusted
to be about 65 nm. The ﬁlm was annealedfor 24 h at 423 K under vacuum. Ethanol,
1-propanol, and 2-propanol were used as
non-solvents.
Figure 1 (a) shows the NR proﬁlesfor the dPMMA ﬁlms under air, ethanol, 1propanol, and 2-propanol. The open symbols denote experimental data and solidlines show best-ﬁtting curves calculated on
the basis of the model scattering lengthdensity (b/V) proﬁles shown in the panel(b), where the abscissa was normalizedwith the initial thickness in air. While thedPMMA ﬁlm was discernibly swollen under all alcohols, the extent was not the sameamong them. Interestingly, the segregationof alcohol molecules was observed at thesubstrate interface for all the cases. The
overall contents of ethanol, 1-propanol and2-propanol in the ﬁlm were 13, 5.7 and 5.7
vol.%, respectively. The solubility parameters for ethanol, 1-propanol, 2-propanoland PMMA are, respectively, 26.0, 24.3, 23.5
and 22.7. Thus, to what extent alcohol
molecules penetrate into the ﬁlm can be
hardly explained only in terms of the solubility parameter. The size of penetrants
should be also taken into account.
References[1]K. Tanaka, Y. Fujii, H. Atarashi, M. Hino,and Nagamura, Langmuir, 24, 296 (2008).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 987- 230 -

JAEA-Review 2013-039

Fig. 1. (a) Neutron reﬂectivity for a dPMMA ﬁlms
under air, ethanol, 1-propanol, and 2-propanol. The
scattering length density proﬁles are shown in (b).
For clarify, each data is off-set by a decade.

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JAEA-Review 2013-039

1-5-37

An Eﬀect of Electromagnetic Wave Treatment on Polymer Diﬀusion
Hironori Atarashi(1), Toshihiko Nagamura(1), Masahiro Hino(2), Keiji Tanaka(1)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2. Resarch
Reactor Institute, Kyoto University, Kumatori, Osaka 590-0494, Japan
Recently, a microwave treatment has
been widely adopted for polymer synthesis because the treatment accelerates the
movement of reactants in the system. The
advantage of the treatment is not only
shortening of the reaction time but alsoeasy controlling of the yield and tacticity.
However, it seems to us that the effectiveness of the microwave treatment on time
evolution of aggregation states in polymer solids has not been discussed yet. In
this study, we examined the microwave effect on interfacial evolution of polystyrene(dPS) bilayers with the aid of neutron reﬂectivity (NR) so that acceleration of chain
diffusion by microwave can be discussed.
Monodisperse PS and deuterated PS (dPS)
were used as samples. Molecular weights
of PS and dPS were 87k and 80k, respectively. A dPS ﬁlm was prepared on a silicon (Si) substrate with a native oxide layer
by a spin-coating method. And, a PS ﬁlm,
which was independently spin-coated ona glass substrate, was mounted onto thedPS ﬁlm by a ﬂoating method. Each ﬁlm
thickness was approximately 50 nm. The
PS/dPS ﬁlms so-prepared were dried under vacuum for 24 h at room temperature,and microwave with the power of 150 W
was irradiated on them under the ambient
atmosphere for 1.5 min and 3 min. Then,the specimens were applied to NR measurements using MINE2 spectrometer.
Figure 1 (a) shows the NR proﬁles for the
PS/dPS bilayer ﬁlms before and after the
microwave treatment. The open symbols
denote experimental data and solid lines
show bets-ﬁtting curves calculated on thebasis of the model scattering length density (b/V) proﬁles shown in the panel (b)of Figure 1. The interface between PS anddPS layers before the treatment was sharp.
The width is basically arisen from the sur-face roughness of the original PS and/or
dPS ﬁlm/s. On the other hand, once thebilayer was treated by microwave, the interface disappeared and the (b/V) value
in the internal region became 3.72 x 104 nm-2, which was almost the middle ofthe (b/V) values for PS and dPS. Thismeans that PS and dPS chains interdiffusedeach other, resulting in the formation of homogenous phase in the ﬁlm. The (b/V)
proﬁles treated for 1.5 min and 3 min were
almost the same. Thus, chain interdiffusionin the bilayer reached a quasi-equilibrium
state even by the 1.5 min.-treatment. Interestingly, the (b/V) value was higher near
the substrate interface than in the interior region. This makes it clear that thedPS component was enriched at the substrate interface in the ﬁlm being in a quasiequilibrium state. The detail mechanism of
how the treatment affects on chain diffusion, especially, a thermal effect induced bysurrounding substance, will be reported in
the near future.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

Fig. 1. (a) Neutron reﬂectivity for a PS/dPS ﬁlmtreated by microwave for 0, 1.5, and 3 min. The scattering length density proﬁles are shown in (b). For
clarify, each data is off-set by a decade.

1-5-37- 233 -

JAEA-Review 2013-039

1-5-38Aggregation Structure and Relaxation Dynamics of Polymers at the Interface with
Water: II. Analysis of Relaxation Dynamics by Neutron Spin Echo
Hironori Atarashi(1), Toshihiko Nagamura(1), Keiji Tanaka(1), Hitoshi Endo(2), andMitsuhiro Shibayama(2)1. Department of Applied Chemistry, Kyushu University, Fukuoka 819-0395, Japan, 2. Institutefor Solid State Physics, The University of Tokyo, Chiba 277-8581, Japan
New tools for tailor-made diagnostics are
generally made from polymers. In theseapplications, the polymer surface is in contact with a water phase. However, despite the importance of detailed knowledgeof the fundamental interactions of polymer interfaces with liquids, such studies
are very limited. We have hitherto studied aggregation structure of poly(methyl
methacrylate) (PMMA) at the interfaces
with non-solvents by neutron reﬂectivity.[1] As a result, the liquid/polymer interfaces were diffuse in comparison withthe air/polymer interface, probably due tointerfacial roughening and the partial dissolution of segments at the outermost region of the ﬁlm. In this study, relaxation
dynamics of PMMA chains at the interfaces
with typical non-solvents such as waterand methanol was discussed on the basisof small angle neutron scattering (SANSU) and neutron spin echo (iNSE) measurements. PMMA particles with diameter ofabout 300-500 nm (MP-2200 produced by
Soken Chemical & Engineering Co., Ltd.)
were used as a sample to increase the scattering volume rather than a ﬁlm. Deuterated water (D2O) and ethanol (CD3OD)
were used as non-solvents. The PMMA
particles mixed with a non-solvent were
ﬁlled into a quartz cell with 2 mm optical length. The sample-to-detector distancewas chosen to be 2 and 12 m.
Figure 1 (a) shows the SANS proﬁlesfor PMMA particles with water, which theincoherent contribution was subtracted, at
25 and 40 °C. The power for the linear relation was approximately 4 for bothcases. Taking into account that the specimen was PMMA particles, the result isquite reasonable. Interestingly, the power

seems to deviate from 4 at q>10-1 A-1 at 40°C. This may indicate that the interface between PMMA and water became broader
with increasing temperature. Figure 1(b)shows the SANS proﬁles for PMMA particles with methanol. In this case, the slope
transformed 4 to smaller once q went beyond 5*10-2 A-1. This means that the interface between PMMA and methanol wasquite diffused in comparison with the caseof water. Then, iNSE measurement wasmade using the same sample. A certain
relaxation was somehow observed both in
the case of PMMA particles with D2O and
CD3OD. The detail analysis for the results
has undergone several revisions.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 986- 234 -

JAEA-Review 2013-039

Fig. 1. Temperature dependence of SANS proﬁles(a) in D2O and (b) in CD3OD.

1-5-38- 235 -

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6 Biology

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JAEA-Review 2013-039

1-6-1
Hydration Level Dependent Protein Dynamics Studied by Neutron Inelastic
Scattering
H. Nakagawa and M. Kataoka
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Water is indispensable for life. In physiological condition most proteins work in thesolvated environment and water molecules on
the protein surface strongly aﬀects the protein dynamics. The dynamical transition of aprotein, evidenced as an inﬂection in atomic
mean-square displacements (MSDs) as a function of temperature, has been observed at 200- 240 K with the hydrated protein [1]. In thisstudy, we measured the hydration level dependent dynamical transition of protein Staphylococcal nuclease by incoherent neutron scattering. The neutron scattering experiments
were performed with the triple axis spectrometer, LTAS, in the JRR-3M reactor in Tokai
with an energy resolution of about 80 μ
eV. The hydration levels of protein samples
are 0.10 to 0.62 (g water/g protein). Insetof ﬁgure shows the temperature dependent
atomic mean-square displacement (MSD) ofprotein with hydration level of 0.62 (g water/g protein). As the temperature increase,
the MSD monotonously increases. At around240 K, the protein shows the sharp rise in the
MSD. This is so called dynamical transition,
which is generally observed with the hydrated
biomacromolecules [1]. The slope of the regression line of the temperature-dependent
MSD is related to the resilience of molecular
structure as a force constant [2]. The equation
is below, d(MSD)/dT=0.00276/k ,where k isforce constant (N/m). Figure shows the hydration level dependent slope. At higher hydration level, slope is larger, which indicatesthat the dynamical transition is enhanced byhydration. It was found that dynamical transition was more signiﬁcant above the threshold hydration level around 0.4 (g water /gprotein). This suggest that hydration water network on the protein surface with fully
hydrated is closely related to the protein dynamics. The dynamical behavior of hydration
原子炉：JRR-3

装置：LTAS(C2-1)

water is coupled with the protein dynamics.
Such a dynamical coupling drives the hydration dependent protein dynamical transition.

Figure 1: The slope of the regression line as a functionof hydration level estimated by temperature dependent mean-square displacement between 250 K and
300 K as shown in inset.

References
1) W. Doster et al. :“Nature”,337, 754(1989).
2) G. Zaccai et al. :“Science”,288, 1605(2000).

分野：中性子散乱（生物）- 239 -

JAEA-Review 2013-039

1-6-2
Neutron Diﬀraction Study of Porcine Pancreatic Elastase under Active
Conditions
T. Tamada, T. Kinoshita1 , T. Ohhara, K. Kurihara, T. Tada1 and R. Kuroki
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Graduate School of Science, Osaka Prefecture University, Sakai, Osaka 599-8531

Porcine pancreatic elastase (PPE) is a serine protease classiﬁed in the chymotrypsin
family that is possibly the most destructive
enzymes having the ability to degrade virtually all of the connective components in the
body. Uncontrolled proteolytic degradation
by pancreatic elastase (EC 3.4.21.36) causes
the fatal disease pancreatitis. We have already determined the complex structure between PPE and its peptidic inhibitor at JRR3 in JAEA by neutron crystallography.1),2)This neutron structure elucidated the tetrahedral intermediate state of catalysis by serine
protease. For further clariﬁcation of catalytic
mechanism of serine protease, we carried out
the neutron diﬀraction analysis of PPE onlyat active conditions (pD8.0).
The single crystals of PPE were prepared under 0.2 M sodium sulfate in acidic condition(pD 5.0) using sitting-drop vapor diﬀusion
method. The crystal was grown to the sizeof 1.3 mm3 for neutron diﬀraction experiment
by repeating macro-seeding trchniques underbasic condition (pD8.0), and then sealed inquartz capillary for the diﬀraction study (Figure 1). Diﬀraction data were collected atroom temperature using monochromatic neutron beam (λ = 2.9 Å) and recorded on a neutron imaging plate on a single-crystal diﬀractometer (BIX-3) at JRR-3 in JAEA. The
crystal of PPE belongs to the space group
P 21 21 21 with cell dimensions of a = 52, b= 58, c = 75 Å. The total rotation ranges of
97.8˚ were covered by 326 still images with
exposure time of 4 h./ﬂame by step scanning method at BIX-3, respectively. Data
were processed with the programs DENZOand SCALEPACK. Data set was integrated
and scaled to 2.3 Å resolution. Data collection and processing statistics are shown in Table 1. Structural analysis is now in progress.
原子炉：JRR-3

装置：BIX-3(1G-A)

Table 1: Data collection and processing statistics

Resolution (Å)
No. of reﬂections
obserbed
independent
Redundancy
Completeness (%)
Mean I /σ(I )R merge

2.3 (2.38-2.30)
14,2308,140
1.7 (1.4)
77.0 (69.6)
8.5 (3.5)
0.116 (0.292)

Production of larger crystals is also proceeding to collect higher resolution data.

Figure 1: Crystal of porcine pancreatic elastase.

References
1) T. Kinoshita, T. Tamada, K. Imai, K. Kurihara,
T. Ohhata, T. Tada, R. Kuroki : “Acta Crystalgr.”, F64, 217 (2008).
2) T. Tamada, T. Kinoshita, K. Kurihara, M. Adachi,
T. Ohhata, K. Imai, R. Kuroki, T. Tada : “J. Am.
Chem. Soc.”, in press.

分野：中性子散乱（生物）- 240 -

JAEA-Review 2013-039

1-6-3
Contrast Variation Measurements of Various Intermediates of Hen Egg White
Lysozyme Amyloid Fibrils
S. Fujiwara, F. Matsumoto and H. Nakagawa
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

In neurodegenerative diseases such as
Altzheimer’s disease and Parkinson’s disease,ﬁlamentous protein aggregates called amyloid
ﬁbrils are thought to be related to pathogenesis of these diseases. Elucidation of themechanism of the amyloid ﬁbril formation isthus important for the development of therapeutic strategies against the amyloid diseases. Moreover, since the amyloid ﬁbrils arefound to be formed by proteins that havenothing to do with diseases, it should be of
considerable help to gain an insight into thegeneric properties of proteins related to themechanisms of folding and stability. It was
found that hen egg white lysozyme (HEWL)
forms the amyloid ﬁbrils in highly concentrated ethanol solution1) . The HEWL-waterethanol system is suitable to study the general 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 three samples: 2 mg/ml HEWL solution in 90% ethanol, 10 mg/ml HEWL solution in 90% ethanol, and 10 mg/ml HEWL solution containing 1mM NaCl in 90% ethanol,
which correspond to the protoﬁlament state,
the state where the lateral association of the
protoﬁlament occurs, and the ﬁnal amyloid
ﬁbril state, respectively. The SANS curves ofthese HEWL solutions, prepared in various
fractions of deuterated solvents, were mea原子炉：JRR-3

装置：SANS-J(C3-2)

sured with SANS-J at the guide hall of thereactor JRR-3M in JAEA, and cross-sectional
Guinier analysis was done to estimate thecross-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 of the
10 mg/ml HEWL solutions were ﬁt with alinear function of 1/(Δρ) while the data of
the 2 mg/ml HEWL solution was ﬁt with aquadratic function. These results imply thatthe protoﬁlament has a low density region in apart of the peripheral region, while the amyloid ﬁbrils have the low density region in acentral region of the ﬁbrils. Detailed analysis
with aid 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).

分野：中性子散乱（生物）- 241 -

JAEA-Review 2013-039

1-6-4
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

Elucidating how a protein is folded into theunique tertiary structure is one of the mostimportant problems in biophysics. 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 folding of 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.
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 takes
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
原子炉：JRR-3

装置：SANS-J(C3-2)

Japan Atomic Energy Agency. The measurements were done with the incident neutrons of
the wavelength of 6.5 Å(λ/Δλ=13.4%). To
cover the Q-range as wide as possible, themeasurements were done at two sample-todetector distances, 6 m and 2.5 m. Figure
1 shows the diﬀerence curve of the SANS
curve of d-rhodanase-GroEL-GroES and thatof h-rhodanase-GroEL-GroEs, corresponding
to the curve arising from rhodanase within
the GroEL-GroES complex. The curve showsthat under the condition where the measurements were done, rhodanase formed large
complexes. It, however, clearly demonstrates
the feasibility of the experiments.

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).

分野：中性子散乱（生物）- 242 -

JAEA-Review 2013-039

1-6-5
Neutron Diﬀraction of Protein Single Crystals in H2 O
S. Fujiwara, T. Ohhara and T. Chatake1
1

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

Neutron scattering and diﬀraction provide
unique information that cannot be obtained
from other methods for structural studies of
biological macromolecules. Because of a large
diﬀerence in the scattering length density ofwater 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) O) due to the diﬀerence in the scat2
tering length of hydrogen (-0.3742 × 10−12cm) and deuterium (0.6671 × 10−12 cm), it ispossible to vary widely the scattering lengthdensity of solvent by changing the fractionof D2 O in the solvent. This ”contrast variation” technique has found wide applications
not only in small-angle neutron scattering but
also in low-resolution neutron crystallography. Application of the contrast variation
technique in neutron crystallography provides
information on individual components in avery large macromolecular complex such as
nucleic acid regions within viruses and nucleosomes, and on disordered components inthe complex such as lipid moiety in lipoproteins and detergent moiety in membrane proteins. 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 of amino acids is estimated because eachamino acid has distinct scattering length density. Furthermore, neutron ﬁber diﬀraction
measurements using the contrast variation
technique obtained the results suggesting thepossibility of distinguishing the static disorder and dynamic ﬂuctuations1) .
To explore such possibility of low-resolution
neutron crystallography using the contrast
variation technique, we started a project of
the contrast variation measurements in theneutron diﬀraction. As a ﬁrst step, we prepared a single crystal of proteins in H2 O, andmeasured diﬀraction patterns.
原子炉：JRR-3

装置：BIX-3(1G-A)

A crystal of RNase A was used in the measurements. The crystal, grown in H2 O solution to the size of about 2 mm3 , belongs
to the space group P21 with cell dimensionsof a = 30.10 Å, b = 38.20 Å, c = 53.21 Å,
α = γ = 90◦ , and β = 108.17◦ . Diﬀraction images were collected at room temperature using monochromatic neutron beam (λ= 2.9 Å) and recorded on a neutron imaging
plate on a single-crystal diﬀractometer (BIX3) at JRR-3 in JAEA. A total rotation rangeof 187◦ was covered by 375 oscillation images
with an exposure time of 1800 sec/image by arotation angle of 0.5◦ . Figure 1 shows an example of the diﬀraction images. The diﬀraction spots out to the resolution of about 2.0
Åwere observed. The data were processedwith DENZO and SCALEPACK. Full data
set out to 2.5 Åresolution was integrated andscaled. The observed reﬂections were merged
into 3364 unique reﬂections with an Rmerge of
0.096 and completeness of 84.3%. Structure
analysis is now in progress.

Figure 1: Example of the diﬀraction patterns collected
at BIX-3.

References
1) S. Fujiwara et al.: ”J. Struct. Biol.” 167, 25 (2009).

分野：中性子散乱（生物）- 243 -

JAEA-Review 2013-039

1-6-6

Enhancement of Lipid Flip-Flop by Membrane Proteins and Transmembrane
PeptidesM. Nakano(A), M. Fukuda(A), M. Miyazaki(A), Y. Wada(A), H. Endo(B)(A)Graduate School of Pharmaceutical Sciences, Kyoto Univ., (B)ISSP-NSL, Univ. of Tokyo
Interbilayer transport and transbilayer
movement of phospholipids are crucial
for cell growth, development and survival, and are controlled by lipid transfer
proteins and translocase enzymes. The
endoplasmic reticulum (ER), in which
phospholipids are newly synthesizedon the cytosolic leaﬂet, maintains membrane symmetry, presumably by ﬂippase
activity, which is bidirectional and energyindependent. On the other hand, theplasma membrane retains asymmetriclipid distribution via aminophospholipid
translocase that mediates the unidirectional transport of phosphatidylserine
and phosphatidylethan-olamine from theectoplasmic to cytoplasmic leaﬂet of the bilayer. Disruption of the asymmetry in cellsby the action of phospholipid scramblaseis involved in apoptosis and is associatedwith increased binding and phagocytosisof these cells by macrophages.
Understanding and control of these lipid
dynamics quantitatively is therefore a key
challenge in biophysics and cell biology.
Although this transbilayer movement oflipids is considered protein-mediated, it isunclear whether it involves a dedicatedﬂippase or the mere presence of proteinsin the ER bilayer. Kol et al. have observedthat peptides that mimic the alpha-helicesof transmembrane proteins can stimulate
ﬂip-ﬂop of ﬂuorescence-labeled phospholipids in liposomes [1], which indicates thatthe ability to catalyze ﬂip-ﬂop in the ER
is not necessarily restricted to one speciﬁc
protein.
We previously demonstrated by SANS
that shorter acyl chain lipid, dimyristoylphosphatidylcholine (DMPC) can
ﬂip-ﬂop in large unilamellar vesicles(LUVs) [2], while longer acyl chain lipid,
1-palmitoyl-2-oleoylphosphatidylcholine(POPC) can not. In this study, similar
experiments were carried out with small
unilamellar vesicles (SUVs) of DMPC,
and POPC LUVs in the presence of atransmembrane peptide.
LUVs consisting of deuterated (D-LUV)
or hydrogenated POPC (H-LUV) were prepared by extrusion method in the presence
and absence of 0.5 mol% a transmembrane
peptide KALP23. DMPC SUVs (D- and HSUV) were prepared by sonication. TRSANS measurement was started immediately after mixing equivalent volume of Dand H-vesicles. Time-course of the normalized contrast was calculated from the scattering intensity.
In the presence of methyl-β-cyclodextrin,
the normalized contrast for POPC LUVs
reached around 0.5 and became constant,which suggests that POPC does not ﬂipﬂop at all. In the presence of KALP23, however, no ﬂip-ﬂop was observed. This result suggests that a mere insertion of transmembrane helices into bilayer does not mediate the lipid ﬂip-ﬂop.
DMPC in SUVs showed faster ﬂip-ﬂop
compared with the same lipid in LUVs.
Curvature of the membranes is consideredto alter the environment of lipids, such as
acyl chain packing and/or headgroup hydration, and affect the lipid dynamics.
References[1] 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.
[2] M. Nakano, M. Fukuda, T. Kudo, H.
Endo, T. Handa, Phys. Rev. Lett. 98 (2007)
238101.

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JAEA-Review 2013-039

1-6-7

Structure and dynamics of β-lactogloblin in alcohol-water mixture
Koji Yoshida and Toshio Yamaguchi
Department of Chemistry, Faculty of Science, Fukuoka University
The secondary and the higher-order
structures of protein are affected by thehydrophilic and lipophilic balance (HLB)
of solvent. In alcohol-water mixture, we
can control the HLB of solvent by changing the composition of alcohol. In fact,alcohol-induced α-helix formation of peptides and proteins is well known and has
been widely used in biophysics and biochemistry. So far, in order to investigate the alcohol effect on the native structure of monomer protein, we have measured the circular dichroism (CD) spectra of chymotrypsin inhibitor 2 (CI2) as afunction of alcohol mole fraction in aqueous mixtures of methanol, ethanol, triﬂuoroethanol (TFE), and hexaﬂuoro-isopropanol (HFIP)[1]. The CD spectra haveshown that the secondary structure of CI2changes from β-strand to α-helical structure at alcohol mole fractions characteristicof the individual alcohols in an order of
HFIP > TFE > ethanol > methanol. In thepresent study, small-angle neutron scattering (SANS) and neutron spin echo (NSE)measurements were performed on alcohol
aqueous solutions of β-lactogloblin (β-Lg)
in order to investigate the alcohol effect on
the higher-order structure and dynamics ofthe protein.
The β-Lg powder (>90 %) was
lyophilized in D2 O to exchange labilehydrogens with deuterons.
The β-Lg
powder was resolved in D2 O with deuterated hydrochloric acid and stirred with avortex mixer for 30 s. The concentrationof DCl was adjusted to 0.1 M in the ﬁnal
solution. And then alcohols were added
to the solution up to a desired alcohol
concentration and stirred with a vortex
mixer for 30 s. Deuterated alcohols usedwere methanol-d4 , ehtanol-d6 , 2-propanold8 , and 2,2,2-trifuluoroethanol-d3 . In thisstudy, the unit of alcohol concentration isvolume percent.
The wavelength used for small-angle
neutron scattering was 6 Å. The neutron
beam size at the sample position was 7mmφ. A sample solution was kept in aquartz cell of 2 mm path length. The cell
was inserted into a temperature-controlledchamber. The temperature in the chamber was 298K and controlled within ±0.1K.
The distances between the sample and detector were 1 and 4 m, corresponding to
the momentum transfer (Q) of 0.007 - 0.14
Å−1 . The measuring time was 10 min
to 1 h depending on scattering intensity.
Measurements were also made for background, an empty cell, and lupolen used
for intensity normalization. The SANS
data of the sample solutions and the empty
cell were corrected for absorption by usingtransmission data measured, and then theempty cell data were subtracted as background from the data of the sample solutions. Correction for the detector efﬁciency
and normalization to absolute units weremade by using the intensity of lupolen.
The SANS proﬁles of β-Lg in alcoholwater mixtures showed that β-Lg exists as
a monomer at low alcohol concentrations(<30% methanol, <20% ethanol, <20% 2propanol, and <10% TFE). The radius of
gyration (RG ) of β-Lg was calculated with
the Gunier equation. The values of RG
of β-Lg were almost independent of alcohol in these alcohol concentrations. The
CD spectra indicated that the degree of αhelical structure enhanced with the alcohol
addition was less than 20% in these alcohol
concentrations [2]. Hence, β-Lg is likely tostill keep the native structure in these alcohol concentrations. With increasing alcohol
concentration, the large scattering intensity
in a low Q region was observed. The SANS
proﬁle could be ﬁtted with a power function whose exponent was 1.7 independent

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
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JAEA-Review 2013-039

of alcohol. This implies that a homogenous
network of β-Lg was grown. The CD spectra exhibited that the α-helical structure of
β-Lg was dominant in these alcohol concentrations [2].
For the NSE measurements, the wavelength used was 7.3 Å. The scattering vector Q covered was 0.01 - 0.1 Å−1 . The
Fourier time was varied from 0.15 to 15 ns.
The measuring time was 4 to 12 h for each
Q range depending on scattering intensity.
A plate of Grafoil was measured for resolution correction. The sample temperature was 292K and was controlled within±0.3K. The intermediate scattering functions (ISF) of β-Lg at various Q values were
measured in pure D2 O, 20% ethanol-, and
10% TFE- D2 O mixtures. The ISFs wereﬁtted with a single exponential function.
The Q2 dependence of the relaxation rate
in pure D2 O, 20% ethanol-, and 10% TFED2 O mixtures are shown in Figure 1. The
diffusion coefﬁcients (D) were obtained byusing a least-square ﬁtting procedure over
0 < Q2 < 0.01 Å−2 . Hydrodynamic radius(Stokes radius) R H was determined by the
Stokes-Einstein equation. The R H value inpure water (40.2Å) is smaller than that inalcohol-water mixtures (43.4 and 43.1Å in
20% ethanol- and 10% TFE-D2 O mixtures,
respectively). Because the radii of gyration of β-Lg in these solvents are almost
the same as mentioned above, the increasein R H in alcohol-water mixture would notarise from an increase of the Stokes friction. On the other hand, the R H values
obtained from dynamical light scattering(DLS) measurements were almost the sameirrespectively of solvents [3]. This difference would be explained in terms that NSE
would detect internal motion of β-Lg due
to a smaller wave length of neutrons. Thatis, even small addition of alcohol which seldom affects the ternary structure of β-Lg
would retard internal motion of the protein. This is consistent with the results ofmolecular dynamics simulation of a small
peptide in TFE-water mixture [4].
[1] K. Yoshida, J. Kawaguchi, S. Lee, T.
Yamaguchi, Pure Appl. Chem. 80, 1337

(2008).
[2] D. Hong, M. Hoshino, R. Kuboi, Y.
Goto, J. Am. Chem. Soc. 121, 8427 (1999).
[3] K. Yoshida, T. Yamaguchi, unpublished.
[4] M. Fioroni, M. D. Diaz, K. Burger, S.
Berger, J. Am. Chem. Soc. 124, 7737 (2002).

Fig. 1. Q2 -dependence of the relaxation rates of βlactoglobulin obtained from ISF of NSE in aqueous
solutions of 10% TFE and 20% ethanol.

1-6-7- 246 -

JAEA-Review 2013-039

1-6-8

Eﬀect of temperature and pressure on protein dynamics studied by inelastic
neutron scattering
Hiroshi Nakagawa[1], Yasumasa Joti[2], Osamu Yamamuro[2] and Mikio Kataoka[1,3]
JAEA[1], Univ. of Tokyo[2], NAIST[3]Protein structure ﬂuctuates thermally, andthe protein dynamics contributes to the stability and biological function. Protein dynamics has been described from the view
point of the energy landscape. The structural ﬂuctuation accompanies the volume
ﬂuctuation, indicating that protein dynamics should be characterized by the compressibility. Therefore, the effect of pressure as well as temperature on the protein energy landscape is essential for understanding the protein dynamics [1]. Inelastic neutron scattering (INS) is an effective method for studying the protein
dynamics between picosecond and nanosecond time scales. So far the temperature dependence of protein dynamics inthe powder state is well characterized, but
the pressure effect on protein dynamics has
not been studied well. Recently, the gaspressure system has introduced by O.Y.
into the neutron spectrometer, AGNES. We
performed INS experiment with AGNES,
whose energy resolution is 120 μ eV, using Staphylococcal nuclease (SNase) of dehydrated samples at several sets of temperatures and pressures. Ar gas was usedas pressure medium because of the relatively low background. Figures are the INS
spectra at 160 K and 300 K under 1 atm
and 900 atm. At 160 K pressure affects thelow energy dynamics, whereas the vibrational spectrum with high frequency is notaffected by high pressure. In the low energy region, the boson peak was observed,
and the peak shifts to higher frequency athigh pressure, suggesting potential hardening of protein collective modes. At 300 K
and 1 atm, the quasi-elastic scattering appears aside the elastic peak, suggesting onset of the structural relaxation and/or diffusive dynamics. The quasi-elastic scattering signiﬁcantly suppressed at high pres-sure and the boson peak was observed
clearly, indicating that the protein conformation falls into a local minimum on theenergy landscape at high pressure. Anharmonic motions were strongly suppressedby pressure. The anharmonic motions lostat high pressure should contribute to the
biological function. Therefore, INS experiment along the axis of pressure as well asthat of temperature is essential for analysisof the relationship between protein dynamics and function. Furthermore, the systematical studies of protein dynamics by thehigh-pressure INS experiment will open a
new way to analyze the stability and function of the protein originated from the living organism in the deep sea (ex. Why is a
deep-sea ﬁsh alive?) and give an important
insight into the piezo-biology.
1) L. Meinhold et al. : Proc.Natl.Acad.Sci. ,104, 17261 (2007).

Fig. 1. INS spectra at 160 K and 300 K under 1 atm
and 900 atm.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 786- 247 -

JAEA-Review 2013-039

1-6-9

Denaturation of alpha-Crystallin by replacement of amino-acid residue
Masaaki Sugiyama, Norihiko Fujii, Toshiharu Fukunaga and Noriko Fujii
Research Reactort Institute, Kyoto University
We have investigated on the mechanism of the abnormal aggregation of protein with the eye lens protein, α-Crystallin.
Alpha-Crystallin with its molecular weightof ca 800 kDa is a major protein in eye lens.
Native α-Crystallin is a hetero-aggregatewith 20-30 subunits. There are two kinds ofsubunits, αA-Crystallin and αB-Crystallin.
On the molecular level study, Fujii foundthat there exist racemized aspartyl residues(D-Asp) in the abnormal aggregates of αCrystallin of Cataractous and elder eyelens. Therefore, we have supposed theracemization of aspartyl residue should
be a trigger of abnormal aggregation. In
addition, we have also proposed a pathway to Cataract as follows: Under external stresses such as UV irradiation, X-ray
irradiation, low temperature and so on,
aspartyl residues are racemized. The DAsp on the polypeptide chain induces thestrain in the regular folding of the polypeptides and the strain makes the structuraldeformation of the subunits, αA-Crystallin
and/or αB-Crystallin. The aggregates withthese deformed subunits gather and makethe abnormal aggregates.
As the ﬁrst step to prove above the hypothesis, we prepared for two mutant samples of which an aspartyl residue was replaced with an asparagine residue.
Mutant αA-crystallin (Asp → Asn@151)
Mutant αB-crystallin (Asp → Asn@36)
In addition, as a reference, we also prepared for normal αA-crystallin and αBcrystallin. It is espected that asparagine
acid can make racemization more easily
than aspartyl acid.
With these samples, SANS experiments
were perfomed with SANS-U spectrometer.
Figure 1 shows the SANS proﬁles of nromal and mutant αA-crystallins
and those of nromal and mutant αBcrystallins. The structual change of mu-

tant αB-crystallin is larger than that of mutant αA-crystallin. It means that an aspartyl
residue in αB-crystallin plays more important role than that in αA-crystallin.

Fig. 1. SANS proﬁles of nromal and mutant αAcrystallins (a) and those of nromal and mutant αBcrystallins (b).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 874- 248 -

JAEA-Review 2013-039

1-6-10Analysis of the relationship between the dynamics and the structuralpolymorphism of F-actin
S. Fujiwara (A), F. Matsumoto (A), H. Nakagawa (A), T. Oda (B)(A) Japan Atomic Energy Agency, (B) RIKEN SPring8 Center
Actin is one of the most abundant proteins in eukaryotic cells and plays crucial
roles in various aspects of cell motility.
The actin monomers (G-actin) polymerize
to form a helical polymer (F-actin). Flexibility of F-actin has been suggested to beimportant for such a variety of functions.
Understanding the ﬂexibility of F-actin requires characterization of a hierarchy of dynamical properties, from internal dynamics of the actin monomers through domain
motions within the monomers and relative
motions between the monomers within Factin to large-scale motions of F-actin asa whole. As one of the ongoing projects
towards this ultimate goal, we have been
studying the dynamics of actin at pico- tonano-second time range by neutron spinecho (NSE) spectroscopy.
We carried out the NSE experiments on
solutions of F-actin and G-actin in the Qrange between 0.03 Aˆ-1 and 0.2 Aˆ-1 at theFourier time up to 30 nsec during the machine time in 2007, and found that there
are differences in the intermediate functions obtained, from which it was suggested that behavior of the effective diffusion coefﬁcients of G-actin as a function ofQˆ2 corresponds to free diffusion in solution whereas that of F-actin reﬂects the collective motions within F-actin.
Here, as a continuation to the experiments
on G-actin and F-actin, we investigated effects of solution conditions on the dynamics of F-actin. It was shown that the ﬂexibility of F-actin changes corresponding toa variety of the solution conditions (Isambert et al., 1995). In particular, F-actin polymerized in the presence of Mg2+ (Mg2+-Factin) was shown to have a distinct structural conformation and be more ﬂexible
than F-actin polymerized in the presenceof Ca2+ (Ca2+-F-actin), and it was sug-gested that such modulation of the ﬂexibility by Ca2+ and Mg2+ may have important
physiological consequences within the cell
(Orlova and Egelman, 1993). We thus carried out the NSE measurements of Mg2+F-actin and Ca2+-F-actin.
Actin was puriﬁed from rabbit skeletal
muscles. Actin in the presence of Ca2+ orMg2+ was polymerized by adding KCl. Solutions of Mg2+-F-actin and Ca2+-F-actin
were prepared in D2O. The NSE measurements on these solutions were carried out on the NSE spectrometer, iNSE,
run by the University of Tokyo, installedat the guide hall of the research reactor,
JRR-3M, Ibaraki, Japan. The measurements
were done over the Q-range between 0.03
Aˆ-1 and 0.2 Aˆ-1 at the Fourier time up
to 30 nsec. During the measurements, thesamples were kept at 10 °C. The normalized intermediate scattering functions obtained showed that each intermediate function can be ﬁt with a single exponential,from which effective diffusion coefﬁcientscan be estimated, and that there are differences in the decay times of Mg2+-F-actin
and Ca2+-F-actin. It appears that the decay
times of Mg2+-F-actin are somewhat fasterthan those of Ca2+-F-actin, suggesting that
Mg2+-F-actin is more ﬂexible than Ca2+-Factin. This result is consistent with the previous reports. Detailed analysis of the intermediate functions is currently underway.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 896- 249 -

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1.  ୰ ᛶᏊᩓ஘ 7 ᇶ♏≀⌮Ꮫ㺃୰ᛶᏊගᏛ 

1. Neutron Scattering

7 Fundamental Physics㺃Neutron
Optics- 251 -

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JAEA-Review 2013-039

1-7-1

Development of Neutron Interferometer using polychromatic mirrors
M. Kitaguchi(A), M. Hino(A), Y. Seki(B), H. Funahashi(C), K. Taketani(D), H. M.
Shimizu(D)(A)KURRI, (B)Kyoto Univ., (C)Osaka Electro-Communication Univ. (D)KEK
the JRR-3 reactor in JAEA. The beam has awavelength of 0.88nm and a bandwidth of
2.7% in FWHM. In the case of monochromatic beam of MINE2, the polychromatic
mirrors functions at two Bragg angles. Theinterferometer can be constructed at thetwo incident angles. We observed clear interference fringes at the incident angle of
1.14 degree and 1.62 degree, which werecorresponding to the two multilayers in thepolychromatic mirror (ﬁgure 1).
Now we are planning to apply the supermirror for BSEs and to construct the interferometer for pulsed neutrons. We are alsoplanning the experiments using the interferometer as one of fundamental physics
investigations at J-PARC.
[1] M. Kitaguchi, et. al., Phys. Rev A 67
(2003) 033609}polychromatic
mirrorgap layer

Si substrate}polychromatic
mirror

Jamin-typearrangement

neutron counts /60sec

4000
3500
3000
2500
2000
1500
1000

1.14 deg

500
0

phase
shiftercoil

neutron counts /60sec

Neutron interferometry is a powerful technique for studying fundamental physics. A
large dimensional interferometer for longwavelength neutrons has the advantage
to increase the sensitivity to small interactions. Such a kind of interferometer
was realized by using multilayer mirrors.
We demonstrated Jamin-type interferometer for cold neutrons using beam splitting etalons (BSEs), which enables us toalign the four independent mirrors withinrequired precision [1]. The BSE contains
two parallel mirrors. A couple of the
BSEs in the Jamin-type interferometer separates and recombines the two paths spatially. A neutron supermirror is one of
the multilayer with continuous latice constants, which reﬂects the wide range of
the wavelength of neutrons. The BSEs withneutron supermirrors enable us to arrange
Jamin-type geometory of the interferometer for white neutrons. The interferometercan be applied to pulsed neutrons by using the BSEs with supermirrors. Such interferometer increase the neutron counts forhigh precision measurements, for example,
Aharonov-Casher effect. Wevelength dependence of the interaction in the interferometer also can be measured by the time of
ﬂight detection for pulsed neutrons.
As the ﬁrst test we made polychromatic
mirrors. The polychromatic mirror contained two multilayers with the different
latice constants. The lattice constants were
15.8nm and 21.0nm respectively. We fabricated two polychromatic mirrors with intermediate gap layer on the top of Si substrate continuously. This device enabled
us to provide two separated paths of the
Jamin-type interferometer for two wavelength of neutrons.
The experiment has been performed using the cold neutron beam line MINE2 at

3500
3000
2500
2000
1500
1000

1.64 deg

500000.05 0.1 0.15 0.2 0.25 0.3

phase shifter coil current [A]Fig. 1. Interferometer using polychromatic mirrors.
Interference fringes are observed at two incident angles.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 803- 253 -

JAEA-Review 2013-039

1-7-2

Measurement of magnetic diﬀuse scattering from Ni2MnAl
Kouichi Hayashi, Kenji Ohoyama, Tokujiro Yamamoto, and Toetsu Shishido
Insitute for Materials Research, Tohoku University
Neutron holography is relatively local
structural analysis method, which visualize 3D local atomic arrangements aroundselected elements in solids. This technique
is attracted as local structural analysis of
dopants like X-ray and neutron holography, which have been developed in lasttwo decades. However, the photoelectronor X-ray holography has a disadvantagethat they cannot apply to hydrogen systembecause hydrogen dose not emit any ﬂuorescent X-rays and photoelectrons. In orderto overcome this difﬁculty, neutron holography was proposed in 2001. First demonstration of the neutron holography was realized using a single crystal of simpsonite(Al4Ta3O13(OH)) by Sur et al. They measured angular anisotropy of incoherently
scattered neutrons from hydrogen nuclei,
and reconstructed surrounded oxygen nucleus images. In 2004, Cser et al. applied
this technique to a palladium hydride single crystal, and determined the location ofhydrogen in the PdH. We also measured
efﬁciently the neutron hologram of a palladium hydride single crystal using the powder diffrcatometer of HERMES in JRR-3M
reactor, and found the thermal diffuse scattering effect in the measured hologram.
Neutron scattering has mainly two waysof scatterings such as nucleus scatteringand magnetic scattering. Here, in order toinvestigate the effect of magnetic scattering on neutron hologram, we measured
angular anisotropy of incoherently scatterings by Ni in Ni ２ MnAl single crystal
at room temoerature. The present sample
shows ferro-antimagnetic property below
the Nell temperature of 295 K. The incoherent scattering cross section of Ni wasmuch larger than those of Ni and Al. The
single sample of Ni ２ MnAl was grown by
ﬂoating zone method, its size was 6 mm ina diameter and 5 mm in a thickness. Its

microstructure and crystal structure werechecked by SEM and TEM, respectively.
Wavelength of the neutron was 0.182 nm.
Sample was rotated in the range of 0359 with the step of 1 , where rotation
axis was parallel to the incoming beam direction. Neutrons incoherently scattered byNi 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 to 157 . Dwelling time at eachangle was 600 sec. The average neutron intensity at each pixel was about 500 counts.
Figures 1 show the 2D angular distributions of the neutron intensities around thesample at room temperature and 100 K, respectively. The displayed patterns exhibit
strong spots reﬂecting the sample crystal
symmetry, due to thermal diffuse scattering and magnetic diffuse scattering. In
order to extract hologram pattern due topure magnetic scattering, we must measureholograms of Ni ２ MnAl at different temperatures above and below the Nell temperature of 295. Further analysis is now inprogress.

Fig. 1. Fig. 1 2D distributions of neutron intensities
around Ni2MnAl.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 868- 254 -

JAEA-Review 2013-039

1-7-3

A study on reﬂectivity limit of neutron supermirror
M.Hino1 , M.Kitaguchi1 , H.Hayashida2 , T.Ebisawa2 ,R.Maruyama2 , N.Achiwa3 ,Y.Kawabata1
1
KURRI , JAEA2 , Osaka Univ3
Multilayer mirror is one of the most important devices for slow neutron experiments. A multilayer with small d-spacing
and supermirror with large-m are desirable
to enlarge utilization efﬁciency for neutron
scattering experiments. Here m is a maximum critical angle of the mirror in unit ofcritical angle of nickel and Q of nickel (m =1) is 0.215 nm−1 . It is also very important tofabricate high reﬂectivity supermirror evenin low-m. Ion beam sputtering (IBS) technique enables us to fabricate smooth layer
structure with sharp edge. Indeed, we havesucceeded in fabricating m > 5 supermirrors and very small d-spacing multilayerusing ion beam sputtering (IBS) technique,and neutron optics group in JAEA has installed a large IBS machine and is producing supermirror for J-PARC project. In
these reports, the effect of interface roughness and intermixing at each layer boundary in multilayer seems to be less than surface of substrate even in m > 5 supermirrors. In our previous result, the measured
reﬂectivities were well reproduced by thesimple interface roughness model given in
Debye-Waller factor. The surface roughness of ordinary substrate, for example
commercial silicon wafer and ﬂoat glass,is almost larger than 0.4 nm in rms (rootmean-square). The supermirrors were deposited on silicon wafer using IBS instrument installed in the Kyoto University Research Reactor Institute (KURRI).The deposition rates of NiC and Ti were determinedby X-ray and neutron reﬂectometry. The
real and imaginary nuclear potential values of NiC were estimated to be 230 and
0.063 neV, respectively. Those of Ti were 51 and 0.038 neV, respectively. The deposition rates of NiC and Ti were estimatedto be 0.0315 and 0.037 nm/s, respectively.
We have fabricated m = 2.9 NiC/Ti super-

mirror on ordinary silicon wafers in whichsurface roughness are about 0.4 nm by ion
beam sputtering technique. As shown in
the inset of Fig.1, the measured reﬂectivity at m < 2.8 was much better than the
expected theoretical lines with σ=0.3 and
0.4nm. It was well reproduced by the theoretical line with ideal smooth layer structure in which surface and interface roughness is nothing or very little (σ < 0.1). In
case of IBS technique, supermirror reﬂectivity is not restricted with in the simple
surface roughness model. We realized almost theoretical reﬂectivity limit of m = 2.9
NiC/Ti supermirror by ion beam sputtering technique. It is effective for high reﬂectivity low-m supermirror deposited on an
ordinary substrate to increase the numberof layer. It is also useful for realization ofsmall d-spacing monochromator with highreﬂectivity although we have to estimate
the effect of interface roughness with more
realistic model.

Fig. 1. Measured reﬂectivity of m=3 supermirror inwhich number of layers is 650. The solid lines indicate theoretical ones with σ=0, 0.1, 0.2, 0.3 and0.4 nm. The inset is enlarged at high reﬂectivity(R≥ 0.9).

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 903- 255 -

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1. Neutron Scattering- 257 -

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JAEA-Review 2013-039

1-8-1
Develpoment of U-shaped 3 He PSDs for DNA,A New Backscattering Spectrometer at J-PARC
N. Takahashi1 , K. Shibata1 , T. Yokoo1,2 , S. Satoh1,2 and K. Nakajima1
1

2

Neutron Science Section, MLF Division, J-PARC Center
Institute of Materials Structure Science, High Energy Accelerator Reseach Organization (KEK)

Since detectors are one of the most important key components, it is indispensable toevaluate feasibility and performance of new
detectors and related electronics prior to actual construction of instruments. From thispoint of view, in JFY2008, we have continued
to perform R&D of U-shaped 3 He position
sensitive detectors (PSDs), which are planned
to be used at new backscattering spectrometer DNA which will be constructed at BL02 inMaterials and Life Science Experimental Facility (MLF) at Japan Proton Accelerator Research Complex (J-PARC) by using neutron
beam at MUSASI L port.
The U-shaped PSDs are sequentially coupled
detectors. Since one of the both sides of two
independent simple PSDs is connected eachother by a resistance line, no-detectable area,
so-called dead area, can be reduced for oneside, which is corresponding to right side of
Figure 1. Such a contrivance is necessary forbackscattering instrument at pulsed neutron
source facility and BASIS spectrometer at theSpallation Neutron Source (SNS) is also using
this type PSDs already.
We have tested a U-shaped PSD madeby General Electric/Reuter Stokes (GERS)
which is shown in Figure 1. Diameter oftubes and partial pressure of 3 He are 1/2
inch and 7.7 atmospheres, respectively. Neutron beam with wavelength of ∼ 2 A wascollimated into 1mm2 and irradiated the Ushaped PSD which was on a X-Y stage withstepping motor as shown in Figure 2. Applied
voltage was 1.37 kV. Pulse-height spectrum
has shown good neutron/gamma selectivity.
Satisfactory position resolution of 4.0 mm was
obtained. The dead area was evaluated fromneutron sensitivity of the detector (see Figure3) and obtained to be 41 mm.

原子炉：JRR-3

Figure 1: A prototype U-shaped PSD made by GERS.

Figure 2: Experimental setup at MUSASI L port.

Figure 3: Neutron counts as a function of position of
the U-shaped detector.

装置：MUSASI-L(T2-3-1)- 259 -

分野：中性子散乱（装置）JAEA-Review 2013-039

1-8-2
Eﬀect of Interfacial Roughness Correlation on Diﬀuse Scattering Intensity
in a Neutron Supermirror
R. Maruyama, D. Yamazaki, T. Ebisawa, and K. Soyama

Multilayer structure consisting of Ni and
Ti are widely used for neutron optical elements such as supermirrors. The thicknessof the layers of a supermirror is gradually decreased with the number of the layers to increase the eﬀective critical angle, which is expressed by the ratio m of the eﬀective critical angle of the supermirror to that of natural nickel. High-performance supermirrors
allow the realization of focusing systems. Reﬂected neutrons are divided into specular andoﬀ-specular (diﬀuse) components. Although
the specular component contributes to the focused intensity, the diﬀuse component generates background noise around the focal point.
This causes the serious problem of low signalto-noise ratio in focusing systems such purposes as small angle neutron scattering measurement, in which the diﬀuse component
cannot be removed by slits. The suppressionof the diﬀuse component is, therefore, an important problem along with the realization ofhigher reﬂectivity and larger value of m.
There is a technique of adding carbon
atoms to the nickel layer that leads to higher
reﬂectivity that has been demonstrated byseveral groups to be eﬀective in improving thereﬂectivity of the supermirror. The diﬀuse intensity from a NiC/Ti supermirror was foundto be lower than that from a Ni/Ti suppermirror by more than one order of magnitude.
Figure 1 shows the measured diﬀuse intensity
proﬁles from Ni/Ti and NiC/Ti supermirror
with m = 3. This result implies that a highperformance focusing system with a diﬀuse
intensity down to the order of 10−5 for the
specular intensity can be realized by using a
NiC/Ti supermirror. In this study, in order
to discover the mechanism that controls thediﬀuse intensity from a supermirror, we investigated the crystal structures of Ni and NiCmonolayers and interface structures of Ni/Ti
原子炉：JRR-3

装置：SUIREN(C2-2)

Intensity / Arb. unit

J-PARC Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195

10

5

10

4

10

3

10
10
10

2

1

0

-0.008-0.0040.000-1q x / nm

0.004

0.008

Figure 1: Diﬀuse intensity proﬁles from Ni/Ti (•) andNiC/Ti (◦) supermirrors. Solid lines indicate the calculated proﬁles.

and NiC/Ti multilayers1) .
Ni/Ti and NiC/Ti multilayers consisting of
300 layers with a bilayer thickness of 10 nm
were fabricated in order to investigate thecorrelation between the multilayer interfaces.
Since the measured reﬂectivity diﬀerence between these multilayers was very small overthe momentum transfer range up to 2.7 nm−1 ,where the average interfacial roughness wasestimated to be 0.60 nm rms, it can be said
that the interface roughness of the NiC/Ti
multilayer is the same as that of the Ni/Ti
multilayer. The diﬀuse intensity from the
NiC/Ti multilayer was found to be lower thanthat from the Ni/Ti multilayer by more than
one order of magnitude except for the Bragg
condition (qz = 0.645 nm−1 ) as shown in Fig.
2. This result suggests the following explanation of the diﬀuse intensity diﬀerence between
the Ni/Ti and NiC/Ti supermirrors. When amultilayer has a variable bilayer thickness distribution structure, the diﬀuse intensity at every point on the qx -qz plane includes a diﬀuse
intensity component from those layers that do
not satisfy the Bragg condition. That component from the NiC/Ti multilayer is muchsmaller than that from the Ni/Ti multilayer,
which leads to the diﬀuse intensity diﬀerence
between the supermirrors shown in Fig. 1.
In order to verify this explanation, Ni/Ti
分野：中性子散乱（装置）- 260 -

JAEA-Review 2013-039

Intensity / Arb. unit

(a)
10

5

10

4

10

3

10

2

10

1

0

10
-0.010
4

10

3

10

2

10

1

10

0

Intensity / Arb. unit(b) 10-0.0050.000-1q x / nm

0.005

0.010

-0.0010.000-1q x / nm

0.001

0.002

-1

10

-0.002

Figure 2: Diﬀuse intensity proﬁles from Ni/Ti (•) andNiC/Ti (◦) multilayers consisting of 300 layers witha bilayer thickness of 10 nm. Solid lines indicate thecalculated proﬁles. (a) Rocking scan with qz = 0.645
nm−1 . (b) Rocking scan with qz = 0.31 nm−1 .

Intensity / Arb. unit

and NiC/Ti multilayers were fabricated consisting of 350 layers with a bilayer structurein which thicknesses were distributed in therange of 10 ≤ d ≤ 17 nm. Figure 3 shows
the result of the rocking scan with qz = 0.62
nm−1 , which is within the broad Bragg condition distributed in the range of 0.43 ≤ qz ≤0.645 nm−1 . In the previous result for the
10

5

10

4

10

3

10

2

10

1

0

10
-0.010-0.0050.000-1q x / nm

0.005

0.010

Figure 3: Diﬀuse intensity proﬁles from Ni/Ti (•) andNiC/Ti (◦) multilayers consisting of 350 layers with a
distribution of bilayer thickness of 10 ≤ d ≤ 17 nm.
(Rocking scan with qz = 0.645 nm−1 .) Solid lines
indicate the calculated proﬁles.

multilayers without a bilayer thickness distribution, the diﬀerence between the diﬀuse intensity of the two multilayers was very small

under the Bragg condition as shown in Fig.
2(a). However, the diﬀuse intensity from the
NiC/Ti multilayer is much smaller than thatfrom the Ni/Ti multilayer even within the
Bragg condition when the multilayers have bilayer thickness distribution.
In order to investigate the interface structure that controls the diﬀuse intensity fromthe multilayers, the measured diﬀuse intensity proﬁles were compared with the calculations where the perturbation theory based on
the distorted wave Born approximation wasused. Upon diﬀuse intensity measurementof the multilayers without a bilayer thickness
variation, the diﬀerence between the diﬀuse
intensity of the Ni/Ti and NiC/Ti multilayers was found to be dependent on the Bragg
condition. This is closely related to the vertical correlation between diﬀerent interfaces.
From the result of the diﬀuse intensity calculation for the multilayers consisting of 300
layers with a bilayer thickness of 10 nm (Fig.
2), the parameters of the interface structure
were obtained as σ = 0.60 nm, h = 1.0,ξ = 250 and 70 nm, ξ⊥ = 2.0 and 50 nm
for the Ni/Ti and NiC/Ti multilayers, respectively. Here σ is the average interface roughness, h is the Hurst parameter, ξ is the lateral correlation length, and ξ⊥ is the verticalcorrelation length. Using the same parameter
sets, diﬀuse intensity calculations for multilayers consisting of 350 layers with a distribution of bilayer thickness of 10 ≤ d ≤ 17
nm and for the supermirrors with m = 3 werepreformed. The diﬀerence between the diﬀuse
intensity of the multilayers and supermirrors
were well reproduced by introducing the difference in the lateral and vertical correlation
length (Fig. 1 and 3). These results indicatethat a multilayer with a large vertical correlation length and a small lateral correlation
length eﬀectively suppresses the diﬀuse intensity from a supermirror.
References
1) R. Maruyama, D. Yamazaki, T. Ebisawa, and K.
Soyama :“J. Appl. Phys.”, 105, 103527(2009).

- 261 -

1-8-2

JAEA-Review 2013-039

1-8-3
Performance Test of Scintillator-based Small Neutron Detector
K. Sakasai, T. Nakamura, K. Toh, A. Moriai, E. Shooneveld1 and N. Rhodes1
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195
ISIS Science Diﬀraction and Muon Division, RAL, Didcot, OX11 0QX, UK

Figure 2 shows neutron diﬀraction patternof the Ni powder sample after calibration of
scattering angle. After determination of eachscattering angle in the ﬁgure by Gaussian ﬁtting method, lattice spacings of the sample
were estimated. In summary, the detector has
an excellent performance for neutron scattering experiments. New detectors that meet theactual requirements, e.g., a sensitive area of
原子炉：JRR-3

装置：RESA-2(T2-3-2)

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The fabricated detector was designed tohave a small detection pixel with a spatial
resolution of 3 mm. The detector had only
14 pixels to conﬁrm the characteristics suchas neutron detection eﬃciency and gammaray sensitivity. 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
3×107 . The Si monochrometer was used forgeneration of 2.2 Å-neutrons. Figure 1 shows
neutron sensitivity of the detector as a function of the threshold voltage of the ampliﬁer.
One can see that the detector had a neutron
sensitivity of 84 % at a threshold voltage of
250 mV. One the other hand, we have conﬁrmed that the detector had a gamma-ray
sensitivity of 4×10−7 for 1.3 MeV gamma-ray
at the same threshold voltage in the other experiments. After conﬁrmation of fundamental
performances such as output linearity, demonstration experiments for neutron diﬀraction
were carried out at a neutron wavelength of
1.5 Å. In the experiment, Ni powder sample
was used to check the performance.

196 mm×1,000 mm and the secondary ﬂight
path of 2.0 m, for the engineering diﬀractometer, ”TAKUMI”, at J-PARC, were constructed and installed for the ﬁrst commissioning in 2008.

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A small linear scintillation neutron detector
was fabricated and tested at RESA-II. The
detector was originally developed in RAL forthe engineering diﬀractometer, ENGIN-X, at
ISIS. In this paper, some results of the performance test of the detector is described.

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sample.

分野：中性子散乱（装置）- 262 -

JAEA-Review 2013-039

1-8-4
Measurement of Energy Spectrum of Neutron Beam at MUSASI-H Port
K. Toh, H. Yamagishi and K. Sakasai
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195

The high angle MUSASI beam port provides neutron beam with a scattering angleof about 80 degrees. When pyrolitic graphite(PG) is used as a monochromater, however,neutrons with higher harmonic ones will be
generated because of intrinsic characteristicsof PG. To provide neutron energy information
to users who adopt PG as a monochromater,
neutron energy spectrum was measured by a
TOF method.
The experimental setup is schematicallyshown in Fig.1. The neutron signals were
measured by a multi-channel scalar (Turbo
MCS, EG&G Ortec) through an ampliﬁer(570, Ortec) and a single channel analyzer(551, Ortec). Neutron beam was chopped bya chopper and the chopped neutrons were detected by a 3 He detector with a ﬂight path of
0.5 m. The dwell time of MCS was 10 μs.
Measured neutron spectrum is shown in
Fig.2. The TOF time was converted to neutron wavelength according to relationship between TOF time and the ﬂight path. Threestrong peaks at 1.2, 2.0, and 4.0 Å were observed as seen in Fig. 2. No noticeable peaks
was observed above 5 Å. The most intensecomponent was 2.0 Å-neutrons. Note thatthe data were not corrected by the neutron
detection eﬃciency of the 3 He counter.

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原子炉：JRR-3

装置：MUSASI-H(T1-4-6)- 263 -

分野：中性子散乱（装置）JAEA-Review 2013-039

1-8-5
Development of a Multiplet Magnetic Lens System to Focus
a Pulsed Neutron Beam
T. Oku, H. Kira, T. Shinohara, S. Takata, M. Arai, J. Suzuki, H.M. Shimizu1
J-PARC center, JAEA, Tokai, Ibaraki 319-1195
1
KEK, Tsukuba, Ibaraki 305-0801

quadrupole magnet is highly polarized withpolarization degree P > 0.99 4, 5) . The pulsed
polarized neutrons are delivered through theguide ﬁeld and enter the triplet magnetic lenssystem. The spatial intensity distribution of
the neutrons, which transmitted through thetriplet magnetic lens system, were measured
by using a 2d-position sensitive detector 6) .
At ﬁrst, we performed the pulsed neutron
focusing experiments of the triplet magnetic
lens system without changing the spin ﬂipper
state synchronously with the time-of-ﬂight of
the neutrons. The spin ﬂipper states were
ﬁxed during the single measurement. The
measuring conditions are shown in Table 1.
The measured full widths at the half maximum (FWHMs) of the neutron beam focused
onto the detector position are plotted as afunction of the neutron wavelength λ in Fig.
2. It was found that neutron focal wavelengthchanges depending on the spin ﬂipper states.
The focal condition of the magnetic lens basedon the sextupole magnet is determined by themagnet length Lmag and λ as follows:


Lmag
Lmag
h
h
+√
cot √
·
f=
2
2
Gαmn λGαmn λ(1)Here, f is the focal length, h Plank’s constant,
G the coeﬃcient of the magnetic ﬁeld gradi-

As a magnetic lens based on a sextupole
magnet has neutron wavelength-dependent
focusing property, namely chromatic aberration, it has been proposed that the chromaticaberration can be compensated in the pulsed
neutron beam focusing by changing the focusing and defocusing functions of the magnetic lenses of the multiplet magnetic lens system synchronously with time-of-ﬂight of neutrons 1, 2) . In this study, we designed and constructed a triplet magnetic lens system composed of three sextupole permanent magnets
and two spin ﬂippers, and performed a pulsed
neutron beam focusing experiment with thesystem. The design of the system and the experimental results are shown and discussed.
The experimental setup is shown in Fig.1.
We performed a pulsed neutron focusing experiment at the beamline C3-1-2-1 (NOP)of JRR-3 at Japan atomic energy agency(JAEA). The sextupole magnet functions as
neutron focusing and defocusing lens for neutrons with positive and negative spin polarity, respectively 3) . The three sextupole permanent magnets (M1, M2, M3) and two spin
ﬂippers (SF1, SF2) were located in series asshown in Fig. 1. The neutron beam waspulsed by using a chopper, and then polarized by using a quadrupole magnet (Fig.
1). The neutrons which transmit through the
Quadrupole magnet as a polarizer
Slit1(f )Guide field coil

Ma

Spin flipper(SF1)Ma

ens (M1)

Spin flipper(SF2)
Ma
ens
(M2)

ens

2d-PSD(M3)

Neutronbeam

Chopper

215

700

560

1

Llens1=1500

485

L1=2910
Solenoid coil480
Llens1=400

L2=
Llens1=500

Solenoid coilFigure 1: Experimental setup.

原子炉：JRR-3

装置：NOP(C3-1-2-1)

分野：中性子散乱（装置）- 264 -

JAEA-Review 2013-039

In conclusion, we have constructed a triplet
magnetic lens system composed of three sextupole magnets and two spin ﬂippers to focus
a pulsed neutron beam in a wide wavelength
range with same focal lengths. We performed
the pulsed neutron beam focusing experimentwith the system. By choosing the focusing or
defocusing functions of each sextupole magnet
adequately and synchronously with the timeof-ﬂight of the neutrons, we could focus theneutrons in a wavelength range of between λ= 7.4 Å and 10.8 Å with nearly same focal
length. As the application of the magnetic
lens system, it is considered to be applicable
to a neutron focusing device for the FSANS
instruments with pulsed neutrons, since we
can focus the pulsed neutrons in a wide wavelength range so sharply onto the detector byusing it.
Table 1: The states of the spin ﬂippers and functionsof the magnetic lens.

Without synchronous control with time-of-flight
Case 1Case 2
Case 3
Case 430
25
FWHM [mm]ent, α = |μn /mn | = 5.77m2 s−2 T−1 , mn theneutron mass and μn the neutron magnetic
moment (Fig. 3). By changing the statesof the spin ﬂippers at the wavelength λCO
at which the FWHM curves of Fig. 2 crossover, we can satisfy the focal condition for thepulsed neutrons in a wide wavelength range.
Then, we performed the pulsed neutron focusing experiment by turning on and oﬀ thespin ﬂippers SF1 and SF2 synchronously withthe time of ﬂight of the neutrons at the crossover wavelengths λCO1−3 (Fig. 2). The obtained results are shown in Fig. 2. As theresult, the neutron beam size at the detector position were realized to be the narrowest
among the cases 1 to 4. The FWHMs were
kept less than 4 mm between λ = 7.4 Å and10.8 Å (Fig. 2) and the tail of the intensity peak decreased sharply down to the background level with increasing distance from thepeak center. The magnetic lens system is applicable to a focusing geometry small-angle
neutron scattering (FSANS) instrument withpulsed neutrons. In the application, pulsed
neutrons in a wide wavelength range should
be focused with a ﬁxed focal length for eﬃcient utilization of the neutrons. Moreover,the neutrons should be focused on the detector so sharp that the peak tail intensity goes
down to the background level rapidly.

With synchronous control with time-of-flight

20
15
10
5
0

7

8

λCO1 9 λCO2

10 λ

11

CO3

Wavelength [Å]Figure 2: The FWHM of neutron beam focused onto
the detector position as a function of the time of ﬂightof the neutrons.

2f
f
Neutronbeam

Point source

Lmag

Focal point

Figure 3: A schematic layout of a magnetic lens which
focuses the neutron beam with focal length f .

References
1) J. Suzuki et al., the presentation at the International symposium on Pulsed Neutron and Muon
Science, IPS08.
2) T. Oku, et al. :“NIM-A” 600 pp. 100-103 (2009).
3) H.M. Shimizu, et al. :“NIM-A” 430 pp. 423-434(1999).
4) T. Oku, et al. :“Physica B” 397 pp. 188-191 (2007).
5) T. Oku, et al. :“Meas. Sci. Technol.” 19 034011(4pp) (2008).
6) K. Hirota, et al. :“Phys. Chem. Chem. Phys.” 7
pp. 1836-1838 (2008).

- 265 -

1-8-5

JAEA-Review 2013-039

1-8-6
Neutron Beam Focusing with a m= 4 Supermirror on a Precisely Figured
Elliptic Surface
D. Yamazaki, R. Maruyama, K. Soyama, H. Takai1 , M. Nagano1 and K. Yamamura1
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195
Research Center for Ultra-Precision Science and Technology, Osaka University, Osaka 565-0871

We have developed a ultra-precise focusing
mirror combining a high-performance supermirror deposition technique and a very precise surface ﬁguring method. This mirror isa ﬁrst step of developing a focusing mirror
which satisﬁes the following requirements simultaneously: (1)large critical angle of total
reﬂection, (2) high reﬂectivity, (3) low diﬀuse
scattering, (4)large size and (5) precise surface ﬁgure.
The mirror is a one dimensional elliptic mirror of 90 mm (elliptic) × 40 mm (straight). A
fused silica surface was ﬁgured into an elliptic shape with the numerically controlled local
wet etching technique 1) . NiC/Ti supermirror(m= 4) was deposited on the ﬁgured surface
with an ion-beam sputtering technique 2) . A
photo of the mirror is shown in Fig 1.

focusing mirror, which was placed on the sample stage. The slit width was 0.10 mm.
Figure 2 compares the focused, unfocusedand transmit beam intensities measured withtranslating scans of a slit placed at the focal
position. Focused peak width of ∼0.35 mm
and intensity gain ∼6 has been obtained. Diffuse scattering from the mirror was found lessthan 10−3 of the peak intensity.
5

10
Neutron Counts / 10000mon.

1

FocusedTransmit
Incident
BG

4

10

3

10

2

10

1

10

0

10

-6

-4

-2
0
2
Slit3 Position (mm)

4

6

8

Figure 2: Vertical proﬁles measured with 2θ scan.

In conclusion, we have developed a one dimensional focusing mirror which shows a highperformance with a monochromatic beam.
We are now preparing a performance test withwide-band neutron beam. The fabrication
method is readily applied to larger mirror substrates or two dimensional mirrors. Stacked
focusing mirrors could also be fabricated withthese methods.

Figure 1: A elliptic focusing mirror.

The focal length is 1050 mm. The mirror
accepts a neutron beam at a nominal glancing angle of 1.40 deg with acceptance angle
0.12 deg. It, therefore, reﬂects and focuseswide-band neutrons of λ ≥ 3.5Å. Detailed descriptions is found elsewhere 3) .
Focusing of a monochromatic beam was
performed at the SUIREN reﬂectometer 4) .
The neutron wavelength is 3.93 Å. Incident
beam slit was installed at 1050 mm before the
原子炉：JRR-3

装置：SUIREN(C2-2)

References
1) K. Yamamura, Annals of the CIRP, 56, 541 (2007).
2) R. Maruyama, D. Yamazaki, T. Ebisawa, K. Soyama,
Nucl. Instrum. Meth., A600, 68 (2009).
3) K. Yamamura, H. Takai, N. Zettsu, D. Yamazaki,
R. Maruyama, K. Soyama, Opt. Express, 17 6414
(2009).
4) D. Yamazaki, M. Takeda, I. Tamura, R. Maruyama,
A. Moriai, M. Hino, K. Soyama, Physica B (2009),
doi:10.1016/j.physb.2009.06.022

分野：中性子散乱（装置）- 266 -

JAEA-Review 2013-039

1-8-7
Development of a Wavelength-Shifting-Fibre-Based Neutron Imager With a
Fibre-Optic-Taper With a High Spatial Resolution
T. Nakamura, M. Katagiri, K. Toh, K. Sakasai and S. Soyama
Neutron Instrumentation Section, Materials and Life Science Division, J-PARC Center, Tokai
319-1195

A great deal of interest has been paid on
the energy-selective neutron radiogphy at apulsed neutron source. The detector speciﬁcations required in such applications are generally a spatial resolution of less than 100 μm
and a moderate detector eﬃciency with a capability of time of ﬂight measurement. We
have recently developed a compact neutron
image detector for the iBIX instrument in
the J-PARC 1, 2) . The detector comprising aneutron-sensitive scintillator and wavelengthshifting ﬁbers exhibited a spatial resolutionof less than 1 mm with a coverage area of 133
× 133 mm2 with a pulse pair resolution ofa few μs. This paper describes the detector
implementing the ﬁbre optic taper (FOT) in
between the scintillator screen and the WLS
ﬁber ribbons to improve a spatial resolution.
The FOT is a bundle of numbers of ﬁne
glass ﬁbers. The each ﬁber has a taper along
the length, thus the bundle works as an image
magniﬁer. The small-sized FOT that has asmaller-face diameter of 8 mm with a taper ratio of 3.1 is implemented in the demonstrator.
The eﬀective pixel size becomes 0.16 mm since
the side length of the ﬁber is 0.5 mm. The
scintillation light created in the ZnS/6 LiF ispartly collimated and propagated on to theWLS ﬁbers while the light image is enlarged.
Figure 1 shows the measured neutron beam
proﬁle (y direction) when the up half of thedetector was covered with the cadmium mask.
The edge proﬁle was ﬁtted with an edge
spread function. The spatial resolution was
evaluated as 0.33 ± 0.03 mm in full width at
half maximum. The measured edge proﬁle in
the x direction was similar to that in the y
direction. The spatial resolution of the detector was improved by more than a factor
two compared with the original detector that
equipped without a FOT.
原子炉：JRR-3

装置：CHOP(C2-3-3)

The measured spatial resolution of thedemonstrator detector can be understood by
the product of the thickness of the scintillator(0.3 mm) and the inherent spatial resolutionof the original detector (0.8 mm). Further
optimization on the scintillator thickness andthe taper ratio of the FOT would improve a
spatial resolution. The detector also exhibited a temporal resolution of a few μs and amoderate gamma sensitivity of 10−6 as in theiBIX detector.This kind of detector would bequite unique and useful for the neutron transmission measurements at the pulsed neutron
source.

Figure 1: Neutron beam proﬁle measured with theCadmium mask covering up half of the detector.

References
1) M. Katagiri, et. al: Nucl. Instrum. Meth. A, 573,
149(2007).
2) T. Hosoya, et. al: Nucl. Instrum. Meth. A, 600,
217(2009).
3) T. Nakamura, et al: Nucl. Instrum. Meth. A,
604, 158(2009).

分野：中性子散乱（装置）- 267 -

JAEA-Review 2013-039

1-8-8
Development of the Rradiation-resistant Neutron Mirrors for Neutron Guides
I. Tamura, R. Maruyama1 , D. Yamazaki1 , K. Yamamoto, and K. Soyama1
Nuclear Science Research Institute, JAEA, Tokai, Ibaraki 319-1195
1
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195

The neutron guides have been installed in
the ﬁxed plug in JRR-3 to increase the intensity of cold neutron beam. In view of theneutron beam transportation, it is important
to install the neutron guides there. Since they
are near for the cold neutron source, the radiation resistance of the neutron mirror andits substrate become problems. For the reduction in the maintenance cost, we developed the radiation resistance neutron mirror.
Therefore, neutron mirror with the radiation
resistance was fabricated by choosing the substrates with radiation resistance.
Ni mirrors were employed the ion beam
sputtering technique. Substrates whose size
105mm in diameter and 1.5 mm in thickness were selected. The measurements of neutron reﬂectivity of neutron Ni mirrors on the
Soda-lime glass and Glass-like carbon substrate have been carried out at SUIREN1) at
JRR-3 in the Japan Atomic Energy Agency.
The incident neutron wavelength was 3.93Å.
Figure 1 shows the neutron reﬂectivity of
Ni mirror on the Soda-lime glass substrateand ﬁgure 2 shows the neutron reﬂectivityof Ni mirror on the Glass-like carbon substrate. Because reﬂectivities at the eﬀective
critical momentum transfer were almost 1.0,
We succeeded in the manufacturing of Ni mirrors with m=1 on both substrates.
However, the performances of the reﬂectivities of mirrors on the Soda-lime glass substrate were not same as that on the glass-likecarbon substrate. The fringe of reﬂectivity
was observed only in the Ni mirror on the
Soda-lime glass substrate and the thicknessof a Ni layer was 2500∼3000Å clariﬁed fromthe period of it. From the existence of thefringe of reﬂectivity, the performance of thereﬂectivity of the Ni mirror on the Soda-lime
glass substrate is better than that of the Ni
mirror on the glass-like carbon substrate.
原子炉：JRR-3

装置：SUIREN(C2-2)

Figure 1: Neutron reﬂectivity of Ni mirror on the
Soda-lime glass substrate carried out at SUIREN.

Figure 2: Neutron reﬂectivity of Ni mirror on the
Glass-like carbon substrate carried out at SUIREN.

References
1) D. Yamazaki, et al. :“Development of a Neutron
Reﬂectometer SUIREN at JRR-3”, JAEA-Technology
2007-030 (2007).

分野：中性子散乱（装置）- 268 -

JAEA-Review 2013-039

1-8-9
Development of a Hybrid-Anvil Type High-Pressure Device for Single-Crystal
Magnetic Neutron Diﬀraction under 10 GPa
T. Osakabe, H. Yamauchi
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

We developed a hybrid-anvil high-pressure(HA) device for single-crystal magnetic neutron diﬀraction beyond 3 GPa. The device
consists of an opposed pair of a lower sapphireanvil and an upper WC anvil with a hollow inthe center of the culet. The essential point of
the device is the hollow of the WC anvil. A
gasket between the anvils is strongly caught
by the edge of the hollow when the gasket ispressed. As a result, the deformation of thegasket is highly suppressed and the pressure
generation eﬃciency is improved. Obviously,
the hollow can enlarge the volume of the sample chamber. Maximum pressure generated
by the device is 7 GPa 1) .
To increase the maximum pressure up to 10
GPa, we tried three types of the lower anvil
instead of the simple sapphire anvil in the HA
device. One is a sapphire anvil with a thin
diamond cap, another is a sapphire anvil supported by a MP35 alloy, and the other is a
SiC anvil supported by a MP35 alloy. We
found that the modiﬁed hybrid-anvil (mHA)device of the combination of the WC anvil
and the supported SiC anvil could generate
the pressure of 10 GPa at the load of 3.8
tons. Fig. 1 shows a schematic drawing of
the mHA device. Fig. 2 also shows the resultof the pressurization test of the mHA device.
The size of the sample chamber under 10 GPa
was about 1 mm diameter and 0.3 mm height,
which was the same volume as that of the HA
device under pressure and was suﬃcient for
single-crystal magnetic neutron diﬀraction experiments. We succeeded in the single-crystal
magnetic neutron diﬀraction experiments on
the RB2 C2 (R=Dy, Ho) up to 9.6 GPa using
the mHA device.

原子炉：JRR-3

装置：TAS-1(2G)Figure 1: Schematic drawings of a modiﬁed hybridanvil device.

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References
1) T. Osakabe, K Kakurai, D Kawana, K Kuwahara: “J. Magn. Magn. Matt.”, 310, pp. 27252727 (2007).

分野：中性子散乱（装置）- 269 -

JAEA-Review 2013-039

1-8-10
Renewal of a Software and a Data Acquisition System
for the Neutron Reﬂectometer SUIREN
M. Takeda1,2 , D. Yamazaki1,2 , H. Izunome1 and A. Birumachi1
1Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195, Japan
2
J-PARC Center, Tokai, Ibaraki 319-1195, Japan

Neutron reﬂectometry has been widespread
as a powerful and nondestructive technique
to investigate the internal layered structures
now. The new neutron reﬂectometer SUIREN
has been installed at C2-2 beam hole in the
JRR-3 beam hall in 2007 and is now open
to many users. Polarized neutron reﬂectivity
measurements with the full polarization analysis can be performed using this reﬂectometerby inserting the polarized neutron devices1) .
An original software package for controlling the reﬂectometer and a data acquisition system (DAQ) were constructed based on
R
LabVIEW
, and DAQ hardwares of National
R
Instruments
. This system was satisfactory
and worked well. However, we had to wait fora long time to ﬁx minor bugs and to add newcomponents to the reﬂectometer such as additional stepping motors and a one-dimensional
position sensitive detector because a company
who constructed the system was too busy to
manage the system.
Therefore, we decided to use the same software package and DAQ as those used for three
triple-axis spectrometers TAS-1, TAS-2, andLTAS installed at JRR-3. The software package was coded by in-house programmers in
R
JAEA, and ran on HP Tru64 UNIX
on Al-

pha system. This package was ported to Red
Hat Enterprise Linux on x86 based system. A
new DAQ is mainly composed of Multi NT2400 Series which is a commercial product ofLaboratory Equipment Corporation.
A variety of modules and interfaces suchas a stepping motor controller, a MCA, atimer/scaler, a GPIB controller, a mechanicalrelay, and an isolated digital input devices areavailable with a NT-2400 chassis, and thesemodules and devices are controlled by a library software. Figure 1 shows a schematic
diagram of the new system using a workstation operated by the Linux and NT-2400.
We also introduced devices for the neutron
polarization analysis (the 2nd spin-ﬂipper, ananalyzing mirror, and so on) concurrent withthis replacement of the software and DAQ.
We completed the construction of SUIREN
using this new system, and the full polarization analysis of the polarized neutron reﬂectivity can be performed as a routine work on
SUIREN.
References
1) D. Yamazaki, M. Takeda, I. Tamura, R. Maruyama,
A. Moriai, M. Hino, K. Soyama, Physica B 404,
2557 (2009).

stepping motor controler

motor drivers

steping motors

Ethernet (100M)
I/O interface/Relay
8ch timer/scaler
multi channel analyzer

air pads
limit signals
SCA/AMPADC

pre-AMP1/2” neutron detector

Position decoder

AMP

Workstation (for control)
NT-2400

absolute encoder reader

absolute angle encoders

Figure 1: Schematic diagram of new control and data acquisition system for SUIREN.

原子炉：JRR-3

装置：SUIREN(C2-2)

分野：中性子散乱（装置）- 270 -

1D-PSDJAEA-Review 2013-039

1-8-11

A beam divergence correction mirror for neutron resonance spin echo
R. Maruyama A , M. HinoB , H. HayashidaC , M. KitaguchiB , N. AchiwaD , D. Yamazaki A ,T. Ebisawa A , K. Soyama A
A J-PARC Center, Japan Atomic Energy Agency
B Research Reactor Institute, Kyoto University
C Quantum Beam Science Directorate, Japan Atomic Energy Agency
D Graduate School of Science, Osaka University
culated phase where the path length variation is assumed to be corrected in the ﬂight
path between the ﬁrst and the second bootstrap RSF. The calculated phase is in good
agreement with the measured value. This
result demonstrated that a cylindrical mirror effectively corrects a path length variation due to the beam divergence.
(a)Guide end
S1

DC Pi

DC Pi/2

DC Pi/2z

Cylindrical mirror Phase shifter
S2x

Polarizer

2nd bootstrap Analyzer

Guide field

1,350
Intensity / 7,000 s

850

1200
800
400

8 mm

0
0.0

1.0

2.0

3.0

Time / microsec
5000
4000
3000
2000
1000
0

Intensity / 7,000 s

Intensity / 7,000 s

(b)

130
Intensity / 7,000 s

0

6 mm
0.0

1.0

2.0

3.0

1,850

7 mm
0.0

Intensity / 7,000 s

Intensity / 7,000 s

1.0

2.0

3.0

Intensity / 7,000 s

300
200

2 mm
0.0

1.0

2.0

3.0

Time / microsec

Phase / rad

(c)

3.0

2000
1000

5 mm

0
0.0

1.0

2.0

3.0

1500
1000
500

3 mm

0
0.0

1.0

2.0

3.0

Time / microsec

400

0

2.0

3000

Time / microsec

100

1.0

Time / microsec

Time / microsec

4 mm
0.0

y
2,850
mm

5000
4000
3000
2000
1000
0

Time / microsec
2500
2000
1500
1000
500
0

y

2D PSD

1st bootstrap

Intensity / 7,000 s

Neutron resonance spin echo (NRSE) enables us to measure neutron quasielastic scattering with high energy resolution.
Its energy resolution is limited by a path
length variation due to the beam divergence. Neutron focusing technique using
a neutron supermirror can be used to overcome this problem.
A neutron supermirror with cylindricalsurface was fabricated as follows. Supermirror with m = 3 was deposited on Si
wafer with a length of 250 mm, a width of
30 mm, and a thickness of 0.2 mm. When
we assume an incident angle of the central ﬂight path to the cylindrical mirror ofθ = 42 mrad, the object and image distancefrom the center of the mirror of a = b = 500
mm, and the length of the mirror of l = 250mm, the radius of the cylindrical surface of
R = 12 m are obtained from the imaging
equations. The cylindrical proﬁle was produced by numerically controlled machining of an aluminium plate. The back sideof the Si wafer was glued on the cylindrical surface of the aluminium plate using
Araldite epoxy glue.
The experiment was performed using the
JRR-3/MINE1 beam line at JAEA. To investigate the effect of the cylindrical mirror on
the path length variation due to the beam
divergence, MIEZE (Modulation of Intensity by Zero Effort) spin echo measurement
was performed as shown in Fig. 1(a). The
width of the slit (S2) was narrowed to 1
mm to choose a particular ﬂight path fromthe entire beam. Figure 1(b) shows themeasured spin echo signals for the different ﬂight paths chosen by S2. The phaseof the measured echo signals is plotted inFig. 1(c). The solid line indicates the cal-

120
80
40

1 mm

0
0.0

1.0

2.0

3.0

Time / microsec

-0.6
-0.8
-1.0
-1.2
-1.4
-1.6
-1.8
-2.0
1

2

3

4

5

6

7

8

S2 position / mm

Fig. 1. (a) Experimental geometry of MIEZE spinecho measurement. (b) Measured echo signals forthe different ﬂight paths. (c) Phase of the measured
and calculated echo signals.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 705- 271 -

JAEA-Review 2013-039

1-8-12Development of Cubic Anvil type pressure cell for neutron scattering experiments
under pressure
Koji Munakata(A), Kazuyuki Matsubayashi(A), Masakazu Nishi(A), Hiroyuki Kagi(B)and Yoshiya Uwatoko(A)(A)ISSP, Univ. of Tokyo, (B)Grad. Sch. of Sci., Univ. of Tokyo
During last few decades, intensive studies have been performed on strongly correlated electron systems and/or magnetic
materials under high pressure. As a result,with discovery of many interesting physical phenomena at high pressure and low
temperature, new technique and knowhow of high pressure experiments havebeen accumulated. However, in the ﬁeld of
neutron experiments, high pressure technique is less common compared to otherexperiments due to the inevitable difﬁculty,
such is a signiﬁcant decrease in intensity
by absorption and scattering when the neutrons pass through a pressure device thatsurrounds the sample: it is difﬁcult to conduct experiments with reliability and accuracy.
Recently, we have developed small highpressure apparatus for transport and magnetic measurements, a clamp type of palm
cubic anvil cell (PCAC) [1]. This cubic
anvil type pressure apparatus can generate superior hydrostatic pressure to otherhigh pressure apparatus. Then, we optimized anvil material for neutron scattering experiments [2], from tungsten carbide (WC) to ZrO2, relatively transparent
to neutron beams. In this work, pressurization test was carried out at room temperature. For gasket, two types of material are used, a duralumin (A7057) and amesoalite (Meso10) which is Al-based hardmaterial. Glycerol is chosen as a pressuretransmitting medium because of its goodhydrostatic property. A single crystal of
NaCl, 1.5 x 1.5 x 1.5 mm3 in size, was set
in the gasket and pressurized with a hydraulic press. Generated pressures in thegasket were estimated from a compressibility of NaCl by determining a lattice constant from (200) reﬂection at each exter-

nal load. Fig. 1 shows load dependence ofthe proﬁles of (200) reﬂection in θ-2 θ
scan. As shown in the ﬁgure, palpable proﬁles were obtained. No signiﬁcant difference was found between the two materials
of gasket. We conﬁrmed in generating pressure about 7 GPa at the load of 80 ton. We
expect that PCAC will be useful apparatus
in the ﬁeld of high pressure neutron experiments.
[1] Y. Uwatoko et al., Recent Absorbing
Topics in the Research of the Earth’s Interior, 18 (2008) 230. (in Japanese)[2] T. Fujiwara et al., Activity Report on
Neutron Scattering Research: Experimental
Reports 15 (2008) 658.

Fig. 1. Proﬁles of (200) reﬂection of NaCl in θ-2
θ scan at various external loads. At the result of 0
ton, intensity is multiplied by factor of one ﬁfth. The
load of 80 ton is equivalent to 7 GPa.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 996- 272 -

JAEA-Review 2013-039

1-8-13Development of resonance spin ﬂipper with iron yoke
M. Kitaguchi(A), M. Hino(A), Y. Kawabata(A), S. Tasaki(B), H. Hayashida(C), R.
Maruyama(C), T. Ebisawa(C)(A) KURRI, (B) Kyoto Univ., (C) JAEA
yoke around the magnet well.
Test experiments to observe MIEZE signals
with high frequency by using the new RSFs
have been performed using the cold neutron beam line MINE1 at JRR-3 reactor at
JAEA. The beam had the wavelength of
0.81nm and the bandwidth of about 10 % .
Figure 2 shows the MIEZE signal with normalization of the detector efﬁciency. Neutron counts modulated according to thephase of the oscillating ﬁeld of the RSFs.
The effective frequency of the modulation
was 600kHz. The contrast of the signal was
0.58.
This demonstrated the stability and thesmoothness of the magnetic ﬁelds provided by the dipole magnets. MIEZE spectrometer is under ﬁnal process to practical use. We are also continuing to develop
RSF with much higher frequency for NRSE
spectrometer with high resolution. We will
utilize the new system including the new
RSFs for the development of a neutron spinecho spectrometer at J-PARC[3].
[1] F. Mezei, Z. Phys. 255(1972)146.
[2] R. Gaehler, R. Golub, Z. Phys.
B65(1987)43.
[3] Y. Kawabata, et. al., Nucl. Instr. andMeth. A574(2006)1122.

0.3

normalized neutron counts [arb.]

Neutron spin echo (NSE) is one of thetechniques with the highest energy resolution for quasi-elastic scattering by measuring rotation of the neutron spin[1]. In neutron resonance spin echo (NRSE), two resonance spin ﬂippers (RSFs) replace a homogeneous static magnetic ﬁeld for spin
precession in the conventional NSE[2]. An
RSF, which ﬂips the spin of a neutron by exchanging energy between the neutron andan oscillating magnetic ﬁeld, gives the difference of wavenumber between up- anddown-spin components of the neutron. The
relative phase between the two spin components, which is equivalent to spin rotation, is provided by the difference ofwavenumber in the area between the RSFs.
A RSF consists of a static magnetic ﬁeld
and an oscillating magnetic ﬁeld. The staticﬁeld is proportional to the frequency of thethe oscillating ﬁeld. It was quite difﬁcult toprovide the strong static ﬁeld corresponding to the high frequency up to 500kHz byusing air-core coils. New type of RSF has
been developed by using dipole magnet
with iron poles for the static magnetic ﬁeld
(ﬁgure 1). It could provide strong magnetic ﬁeld with less current, however, magnetic ﬂux leak and its surface was not welldeﬁned.
The gap between the two iron poles had
the height of 150mm. The dipole magnet
had the uniform magnetic ﬁeld with thecenter area of 15mm width, 15mm heightand 50mm long. The uniformity was lessthan 10% . About 20mT was measured at
the center of the uniform ﬁeld area with thecurrent of 8A. The magnetic ﬁeld was quite
stable by using the regulated power supply. Temperature of the coil was also stable
for the magnetic ﬁeld which was less than
20mT without any additional cooling system. The return ﬁeld was enclosed by iron

0.25
0.2

0.15
0.1

0.05
0

0

5

10

15

20

25

30

time channel [100nsec]

35

Fig. 1. (Left) RSF with dipole magnet with iron pole.
Fig. 2 (Right) MIEZE signal with 600kHz.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 760- 273 -

JAEA-Review 2013-039

1-8-14Magnetic Imaging with Neutron Spin Interferometry
Yamazaki D., Hayashida H., Ebisawa T., Maruyama R., Soyama K., Takenaka N.a ,Kageyama M.b , Tasaki S.b , Hino M.c , Kawabata Y.c , IIkura H., Yasuda R., Sakai T.,
Matsubayashi M.
Japan Atomic Energy Agency, a Kobe University, b Kyoto University, c KURRI
Stress-induced magnetization change in
Permalloy foils was observed using neutron spin interferometry.
Without samples in a spin interferometer, phases and visibilities of interference
patterns are stable and almost ﬁxed to theirinitial values. If a sample which has magnetic ﬁeld B is placed or a ﬁeld B is applied in the interferometer, the ﬁeld rotates neutron spin around itself and consequently gives rise to phase shifts andvisibility damping. By analyzing phaseshifts and visibility damping, we can obtain both amplitude and direction of ﬁeld.
In addition, 2-dimensional ﬁeld distributions can be observed by measuring interference patterns with a position sensitive
detector (PSD) and analyzing phase shifts
and visibility damping at each pixel of the
PSD. In our experiment, we utilized a 2dimensional PSD with 6 Li scintillator glass.
We prepared three Permalloy foils(A,B,C) of 100 μm in thickness. The foil
A and B were stressed by bending andstretching them just once. The angles ofbent were different for the two foils, 45
degree for foil A and 180 degree for foil B.
The foil C was as is.
A foil was placed vertically in the interferometer and illuminated by monochromatic (8.8 Å) neutron beam of 25 mm (H) ×1 mm (W). As for foils A and B, they wereplaced so that the bend lines are horizontal.
The ﬁgure shows the phase shifts and relative visibilities of foil A and B as functions of vertical position. The red lines
show data from foil A and the blue lines
foil B. Phase shifts are obtaind by subtracting phases of foil C and relative visibilities
by dividing by visibilities of foil C.
It is seen that all lines have a dip at 16.5mm, where the bend line exists. The dips

mean magnetization changes, in amplitude
and direction, at the bend lines of Permalloy foils. The fact that Foil B, bent withthe higher angle, shows the deeper dips inphase and visibility might show the stressdependence of the magnetization change.
We have also obsereved phase shifts andvisibility damping due to a magnetic ﬁeld
induced by two parallel electric currents.
Detailed analysis of these data is now underway and the results will appear elsewhere.
In summary, we showed the capabilityof neutron spin interferometry to identify
magnetic ﬁeld and magnetization distribution. It could be used to explore the current distribution in fuel cells, magnetization properties of ferromegnetic foils andother applications.

Fig. 1. (A) Phases and (B) Visibilities as functionsof vertical position : (Red) 45deg-bent permalloy(Blue) 180deg-bent permalloy

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 789- 274 -

JAEA-Review 2013-039

1-8-15A new MIEZE technique for investigation of relaxation on magnetic nanoparticles
M. Hino1 , H.HAYASHIDA2 , M.Kitaguchi1 , N.Achiwa3 , Y.Kawabata1
KURRI1 , JAEA2 , Osaka Univ.3
In the MIEZE, sample is placed after the
analyzer and there are no optical components between sample and detector. Therefore, the MIEZE spectrometer can be applied to small angle neutron scatteringand neutron reﬂectometry. The contrast
of MIEZE signal can be observed without
reduction even in magnetic scattering although the contrasts of NSE and NRSE areless than half. However, in general, it is noteasy for simple MIEZE setup to separate
magnetic and nonmagnetic ﬂuctuations ofmagnetic nanoscale particles since it measures the both intensities of qausielastic
scattering, simultaneously. We propose a
new MIEZE technique which is to set a second analyzer and an additional π ﬂipper,
in order to separate the magnetic and nonmagnetic quasielastic scattering intensities.
We succeeded in observing the superparamagnetic ﬂuctuations of magnetite particles in ferroﬂuid by using the new technique(Fig.1)[1]. Magnetic ferroﬂuid consists of magnetite particles and solvent(heavy water). The magnetite particles
with a diameter on the order of 10 nm arecoated by oleic acid. There are two kindsof dynamical mode in magnetite ferroﬂuid.
One is Brownian diffusion mode of magnetite particles and the other is superparamagnetic ﬂuctuation which is a relaxationof magnetic moment in magnetite particles.
Both relaxation time depends on particle
size and temperature. The Brownian relaxation time of the particle with the diameter 10 nm is reported to be longer than 2
ns which is out of measurable Fourier time
range in this MIEZE experimental setup.
On the other hand, the relaxation time ofsuperparamagnetism (Neel) is much fasterthan the Brownian relaxation time. We
tried to observe the effect of relaxation onsuperparamagnetism. Here MIEZE signal
is sensitive to the path length dispersion in

neutron trajectories from sample to detector. We estimated instrumental resolutionfunction of the MIEZE spectrometer by using Monte Carlo(MC) simulation. The contrasts from nuclear scattering were well reproduced by MC simulation. On the other
hand, these contrasts from magnetic scatterings were almost less than half of nuclear scattering ones.It is clear that the superparamagnetism relaxation contributes
to reducing the contrast of MIEZE signal
from magnetic scattering.
[1]H.Hayashida, M.Hino, et.
al.,
Nucl.Inst.Meth.A600(2009)56.

Fig. 1. Contrasts of MIEZE signals of nuclear (opencircles), magnetic (open triangles) scattering withthe ferroﬂuid and resolution functions at (a) τ= 0.3,(b)τ =0.8, (c)τ= 1.6 nsec as a function of Q, respectively.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 900- 275 -

JAEA-Review 2013-039

1-8-16Development of Cubic Anvil type pressure cell for neutron scattering experiments
under pressure
Koji Munakata, Kazuyuki Matsubayashi, Masakazu Nishi and Yoshiya Uwatoko
ISSP, Univ. of Tokyo
During last few decades, intensive studies have been performed on strongly correlated electron systems and/or magnetic
materials under high pressure. As a result,with discovery of many interesting physical phenomena at high pressure and low
temperature, new technique and knowhow of high pressure experiments havebeen accumulated. However, in the ﬁeld of
neutron experiments, high pressure technique is less common compared to otherexperiments due to the inevitable difﬁculty,
such is a signiﬁcant decrease in intensity
by absorption and scattering when the neutrons pass through a pressure device thatsurrounds the sample: it is difﬁcult to conduct experiments with reliability and accuracy.
Recently, we have developed small highpressure apparatus for transport and magnetic measurements, a clamp type of palm
cubic anvil cell (PCAC) [1]. This cubic anvil
type pressure apparatus can generate superior hydrostatic pressure to other highpressure apparatus. Then, we optimized
anvil material for neutron scattering experiments [2], from tungsten carbide (WC)to ZrO2, relatively transparent to neutron
beams. In this work, pressurization test
was carried out at room temperature. For
gasket, two types of material are used, aduralumin (A7057) and a mesoalite which
is Al-based hard material. Glycerol is chosen as a pressure transmitting medium because of its good hydrostatic property. A
single crystal of NaCl, 1.5 x 1.5 x 1.5 mm3 insize, was set in the gasket and pressurizedwith a hydraulic press. Generated pressures in the gasket were estimated froma compressibility of NaCl by determining
a lattice constant from (200) reﬂection ateach external load. Fig. 1 shows load dependence of the proﬁles of (200) reﬂectionin θ-2 θ scan. As shown in the ﬁgure, palpable proﬁles were obtained. No signiﬁcant difference was found between the twomaterials of gasket. We conﬁrmed in generating pressure about 7 GPa at the load of
80 ton. We expect that PCAC will be useful apparatus in the ﬁeld of high pressure
neutron experiments.
[1] Y. Uwatoko et al., Recent Absorbing
Topics in the Research of the Earth’s Interior, 18 (2008) 230. (in Japanese)[2] T. Fujiwara et al., Activity Report on
Neutron Scattering Research: Experimental
Reports 15 (2008) 658.

Fig. 1. Proﬁles of (200) reﬂection of NaCl in θ-2
θ scan at various external loads. At the result of 0
ton, intensity is multiplied by factor of one ﬁfth. The
load of 80 ton is equivalent to 7 GPa.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 974- 276 -

JAEA-Review 2013-039

1-8-17Development of pixel detector for ultra-cold neutrons
Y. Kamiya(A), S. Kawasaki(B), G. Ichikawa(B), S. Sonoda(B), S. Komamiya(A)(B), M.
Hino(C), M. Kitaguchi(C), T. Sanuki(D)(A) ICEPP, The Univ. of Tokyo, (B) Graduate School of Science, The Univ. of Tokyo, (C)KURRI
Kyoto Univ., (D)Graduate School of Science, Tohoku Univ.

The ionizing particle converted from theneutron makes a cluster of charged up pixels distributing around an incident point.
Charge sum corresponds to the particle’s
kinematic energy and an weighted centerof the pixels is a good estimation of thepoint. Distribution of the charge sum has
two edges that correspond to the initial energies of the emitted particles (monochromatic), and has tails to the low energy region that represent an energy loss when theparticle transmits through the converter
and a thin insensitive volume on the CCD.
To separate signal events from a background or thermal noise, we apply a cut
to the charge sum distribution. The threshold corresponds to 0.15 MeV energy de-posit. The detector was set on the sample stage which continuously move rightand left in horizontal to be irradiated uniformly. Detector efﬁciency was measured
to 1.7%(0.3%) with Boron(Lithium) based
converter by comparing with the 3He reference detector. Uniformity was evaluatedto less than 3% over the sensitive area. Spatial resolution was estimated by analyzing edges of shadow of the Gadolinium
neutron mask, which is located in front of
the detector surface. Fig.1 shows a neutron distribution taken with the Boron converter. By ﬁtting with error functions foreach edges, the spatial resolution was estimated to 3 microns.
In conclusion, we measured basic performances of the CCD-based pixel detector using the cold neutron beams. The results show that the detector has a ﬁne spatial resolution and enough uniformity. Detector with Boron based converter shows
better performance than that with Lithium
based converter.
Neutrons

CountsA CCD-based pixel detector for ultracold neutrons has been developed. The
detector consists of a back-thinned CCD(S7170-0909, Hamamatsu Photonics K. K.)
with a thin neutron converter directly deposited onto the sensor surface. The active
area is 12.3 x 12.3 mmˆ2 (512 x 512 pixels of 24 x 24 microns). Two nuclear reactions, 10B(n,alpha)7Li and 6Li(n,alpha)3H,
are considered for converter design, wherestrongly ionizing particles are emitted via
those reaction. The thicknesses for theboron based and lithium based converters
are both decided to be 200 nm in consideration of conversion efﬁciency and production easiness. They are sandwiched between titanium layers of 20 nm thickness toprevent oxidizing and crumbling. We used
the Neutron Mirror Fabrication System at
the KURRI to make the detectors with theconverter. Here we report about detection
efﬁciency, uniformity and spatial resolution which were measured using cold neutron beams supplied at the MINE2 line.

Gadolinium Mask
800

600

400

200
0

100

200

300

500
400
Horizontal (microns)

Fig. 1. Neutron distribution. Red line shows an ideal
shadow of the Gadolinium mask. Black line shows
the ﬁtted distribution. Spatial resolution of 3 microns is measured.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 745- 277 -

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JAEA-Review 2013-039

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1.  ୰ ᛶᏊᩓ஘ 9 ㉸ఏᑟ⌧㇟ 
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1. Neutron Scattering- 279 -

9 Superconductivity

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JAEA-Review 2013-039

1-9-1
Structural Analysis on Fe-Based Superconductors, PrFeAsO1−x Fx and
PrFeAsO1−y
K. Kodama1,2 , M. Ishikado1,2 , F. Esaka3 , A. Iyo4,2 , H. Kito4,2 , H. Eisaki4,2 and S. Shamoto1,2
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
JST, Transformative Research-Project on Iron Pnictides (TRIP), Tokyo 102-0075
3
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195
4
Nanoelectronics Research Institute, AIST, Tsukuba, Ibaraki 305-8562

Powder diﬀraction data were collected using the high-resolution powder diﬀractometer (HRPD) at room temperature. Rietveld
analysis was performed by using the program
RIETAN-2000.3) Typical diﬀraction pattern
and ﬁtted result are shown in Fig. 1. The occupancy at O (O1−x Fx ) site is reﬁned in theanalysis and F-concentration is determined by
the secondary ion mass spectrometry in order to determine the valence of Fe-ion. The
lattice canstants, a and c of PrFeAsO1−x Fx
and PrFeAsO1−y , are plotted against the Fevalence in Fig. 2. The lattice constant a (c)of PrFeAsO1−y is larger (smaller) than thatof PrFeAsO1−x Fx even for the parent compounds with Fe-valence of ∼ +2. It is due tothe diﬀerence of the sample preparation condition; under high pressure for PrFeAsO1−y
原子炉：JRR-3

装置：HRPD(1G)

9000

PrFeAsO0.9 F0.1
R. T.

8000
7000
6000
5000
4000
3000
2000
1000
0
10

20

30

40

50

60

70

80

90

100

110

120

130

140

150

160

2 /°

Figure 1: Powder diﬀraction pattern and the result of
Rietveld analysis on PrFeAsO0.9 F0.1 .

c (Έ)

8.62
8.61

(a)

PrFeAsO 1-x Fx
PrFeAsO 1-y

8.60
8.59

3.985



(b)

a (Έ)

Among Fe-based superconductors, a superconductivity in so-called 1111-system is induced by substituting ﬂuorine for oxygen orby oxigen deﬁciency for parent compound
RFeAsO (R:rare earth elements). 1, 2) Generally, it is considered that above two eﬀects
reduce the valence of Fe-ion from +2 and dope
electrons, resulting in the superconductivity.
However, comparing the phase diagram of
the F-substituted system with that of the Odeﬁcient system, the superconducting transition temperature (Tc ) is not scaled by the Fevalence, indicating that the Fe-valence is notunique parameter for the superconductivity.
The atomic substitution and deﬁciency alsochange structural parameters, which modify
the electric state and may induce the superconductivity. Then we have performed thestructural analysis on neutron powder diﬀraction data of PrFeAsO1−x Fx and PrFeAsO1−y ,including parent compounds.

Intensity

2

3.980
3.975
3.970

1.70

1.75

1.80

1.85

Fe valence

1.90

1.95

2.00

Figure 2: The lattice constants, (a) a and (b) cof PrFeAsO1−x Fx and PrFeAsO1−y with tetragonal
structure are plotted against the valence of Fe-ion, byclosed and open circles, respectively.

and in a quartz tube sealed in vacuum for
PrFeAsO1−x Fx . This result suggest thatthe diﬀerence of structural parameters modiﬁng the electric state causes the diﬀerenceof the Tc -Fe-valence phase diagram between
PrFeAsO1−x Fx and PrFeAsO1−y .
References
1) Y. Kamihara, et al. :“J. Am. Chem. Soc.”, 130,3296 (2008).
2) H. Kito, H. Eisaki, and A. Iyo :“J. Phys. Soc.
Jpn.”, 77, 063707 (2008).
3) F. Isumi and T. Ikeda :“Mater. Sci. Forum”, 321-324,
198(2000).

分野：中性子散乱（超伝導）- 281 -

JAEA-Review 2013-039

1-9-2
Magnetic Excitations in LaFeAsO1−x Fx Superconductors
S. Wakimoto1,2 , K. Kodama1,2 , M. Ishikado1,2 , M. Matsuda1,2 , R. Kajimoto2,3 , M. Arai2,3 ,K. Kakurai1,2 , A. Iyo2,4 , H. Kito2,4 , H. Eisaki2,4 , and S. Shamoto1,2
1

Quantum Beam Science Directorate, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
2JST, Transformative Research-Project on Iron Pnictides (TRIP), Tokyo 102-0075
3
J-PARC Center, Japan Atomic Energy Agency, Tokai, Ibaraki 319-1195
4
Nanoelectronics Research Institute, National Institute of Advanced Industrial Science and Technology,
Tsukuba, Ibaraki 305-8562

The recently discovered Fe-pnictide superconductor LaFeAsO1−x Fx has provided aunique opportunity to study the high temperature superconductivity other than the
cuprates. 1) Band calculations indicate cylindrical Fermi surfaces at Γ- and M-points.
From the early stage of the Fe-pnictide superconductor research, many authors havepointed out the importance of spin ﬂuctuations arising from the Fermi surface nesting between the two points in realizing thesuperconductivity. In fact spin ﬂuctuations
have been observed as signiﬁcant inelastic
neutron scattering for the 122-type superconducting compounds, Ba1−x Kx Fe2 As2 2) showing a resonance behavior. On the other hand,
the NMR study of the LaFeAsO1−x Fx system shows dramatic decrease of spin ﬂuctuations near ω = 0 in superconducting compositions. 3)

surprise, it is comparable to that of the nondoped LaFeAsO. These facts suggest that theantiferromagnetic spin ﬂuctuation remains indeep inside the superconducting regime, implying the importance of spin ﬂuctuation inthis system. In addition, we have observedthat the magnetic intensity at ∼ 11 meV increases below ∼ 30 K, consistent with the resonance behavior. More detailed study of doping dependence is now in progress.
100

LaFeAs(O,F)ω = 11 meV

80
60
40
20
0
0

0.02

0.04

0.06

0.08

0.1

0.12

To reconcile these facts, systematic studyof low energy spin ﬂuctuation (ω ≤ 15 meV)has been performed using polycrystalline
LaFeAsO1−x Fx with nominal compositions
x = 0, 0.05, 0.075, and 0.10 (Tc = 0, 25, 25,
and 29 K, respectively). High-quality polycrystalline samples were synthesized by solidstate reaction. 25 g for each composition wasused for inelastic neutron scattering experiments at TAS-1 and TAS-2.

Figure 1: Doping dependence of q-integrated dynamical spin susceptibility χ”(ω) measured at 11 meV.
The data at x = 0 is measured at just above the Néeltemperature where the spin ﬂuctuation becomes maximum. The other data are measured at 4K.

Figure 1 shows doping dependence of theimaginary part of dynamic spin susceptibility χ”(ω) at 11 meV. In contrast to the dramatically diminished magnetic ﬂuctuation observed by NMR, the cross section exclusively
at 11 meV observed by neutron inelastic magnetic scattering decreases little with doping inthe superconducting compounds and, to our1) Y. Kamihara, T. Watanabe, M. Hirano, and H.
Hosono, J. Am. Chem. Soc. 130, 3296 (2008).
2) A. D. Chirstianson, E. A. Goremychkin, R. Osborn, S. Rosenkranz, M. D. Lumsden, C. D. Malliakas, I. S. Todorov, H. Claus, D. Y. Chung, M.
G. Kanatzidis, R. I. Bewley, and T. Guidi Nature
456, 930 (2008).
3) Y. Nakai, K. Ishida, Y. Kamihara1, M. Hirano,and H. Hosono, J. Phys. Soc. Jpn. 77 073701(2008).

原子炉：JRR-3

F doping x

References

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JAEA-Review 2013-039

1-10-1
Behavior of Crack Growth of Austenitic Stainless Steels
under Decrease in Stress
H. Ogawa, I. Ioka and M. Yamamoto
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195

It has been shown that the crack growthcaused by stress corrosion cracking (SCC),
which is located near welded parts at primaryloop recirculation system’s pipes of BWRs, isinhibited. It seems that this inhibition arises
from the reduction of residual stress as thecrack growth. The residual stress becomes a
key factor to control the crack growth. Therefore, it is important to measure residual stressaround the crack. The residual stress using
RESA was measured to clarify the relationship between the crack growth and the residual stress.
The specimens with a crack induced by
fatigue test were prepared. The specimens
were type 316L stainless steel (SS) with highstress at crack tip. The specimens were subjected to heat treatment (850Cx1h, 30%CW).
The stress at the crack tip was generated
by a taper pin as shown in Fig.1. The estimated initial stress intensity factor (K) is√
about 50 (MPa m). The SCC test for crack
growth is conducted in high temperature water (288C, 7.5MPa, saturated dissolved oxygen) for 1000hs. The fracture surface ofspecimen was observed by SEM after SCC
test. Lattice constants corresponded to residual stress were measured along the line of theligament using RESA.
The stress around the crack tip was compared between before SCC test and after SCC test . The result of type 316L SS
was shown in Fig.2. It is found that SCC
enhanced the growth of crack in type 316L
SS. The stress at crack tip was not clearlychange, though the propagation of crack was
estimated about 1mm. Fig.3 shows fracturesurface of type 316L SS after SCC test. The
mode of crack was transgranular (TGSCC)
and the top of crack was not ﬂat. After
SCC test, K corresponded to residual stress
was calculated from the load yielded taper
原子炉：JRR-3

装置：RESA-2(T2-3-2)

pin. The calculated K was a decrease in
65% against the initial K. The residual stresscalculated by K was diﬀerent from that by
RESA. The diﬀerence may be attributed to
the non-uniformity of crack propagation orvoxel size (2x2x1mm).

Figure 1: Taper-pin type CT specimen.

Figure 2: Comparison of lattice constant in type 316L
SS between before and after .

Figure 3: Fracture surface of type 316L after SCC test.

分野：中性子散乱（残留応力）- 285 -

JAEA-Review 2013-039

1-10-2Stress Measurement of Large Scaled Welded Tube
Using Neutron Diﬀraction Technique
H. Suzuki, J. Katsuyama1 , T. Tobita1 and Y. Morii
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
1
Safety Research Center, JAEA, Tokai, Ibaraki 319-1195

Residual stress distributions near weld lineof an austenitic large scaled butt-welded tube
(500 mm diameter, 760 mm length and 28 mm
wall thickness) were measured using the neutron diﬀraction technique to evaluate eﬀects
of crack propagation and repair welding on
the residual stress distribution. The throughthickness distribution of residual stresses were
measured at a position 12.5 mm transverse
away from the weld center using the engineering diﬀractometer, RESA, in the JRR-3 at theJapan Atomic Energy Agency. Two slots (50mm x 150 mm) were machined on the weld
line at 180 deg around the circumference fromthe centre for minimizing the neutron path
length. The lattice constant in stress-free condition was measured using a standard sample
cut from the remaining material obtained after machining the slots. Lattice strains of the
311 reﬂection were measured to avoid the intergranlar eﬀect caused by the accumulated
thermal plastic strain due to welding.
Figure 1 shows changes in residual stress
distributions before and after slitting and repair welding. In as-welded tube, typical residual stress distributions were observed and it
agreed well with the stress distributions calculated by the numerical simulations reported
in previous studies. After machining the slit
with the size of 30 mm length, 10 mm depth
and 0.5 mm width at a position 12.5 mm
transverse away from the weld center on theinside wall of the tube, the residual stresses
in the axial and the hoop directions were released in the part of the slit. On the other
hand, the residual stress distributions after
the repair welding on the outside wall weresigniﬁcantly changed compared with the original stress distributions before repair welding.
Tensile residual stresses were observed after
the repair welding and compressive stresses
原子炉：JRR-3

装置：RESA(T2-1)

were disappeared at all positions in all three
directions. Tensile residual stresses generated
on the inside wall might encourage generationof the stress corrosion cracking, and the tensile residual stresses generated in the middle
might drive the crack propagation. Therefore,
the repair welding would have an inﬂuence onenhancement of crack propagation.
In this study, we indicated that the neutron
diﬀraction technique is useful and powerfultool for measuring residual stress distribution
in the large scaled mechanical components.
This research project has been conductedunder the research contract with the Japan
Nuclear Energy Safety Organization (JNES).

Figure 1: Change in residual stress distributions before and after slitting (a) and repair welding (b).

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JAEA-Review 2013-039

1-10-3
Strain Measurement in Rebar in Reinforced Concrete
by Neutron Diﬀraction
H. Suzuki and K. Kusunoki1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Department of Architecture, Yokohama National University, Yokohama, Kanagawa 240-8501

It is typical method to measure the strains
on a rebar in a reinforced concrete using
strain gauges in the structural engineeringﬁeld in order to evaluate the bond condition
between rebar and concrete. However, waterproof treatment and wiring of the strain
gauges around the rebar would aﬀect the bondcondition. Therefore, the neutron diﬀraction
technique might be useful for measuring thestrains on the rebar in the reinforced concrete
without any eﬀects of the bond condition. In
this study, a size of anchorage zone was evaluated by measuring strain distributions in therebar under pull-out loading.
Figure 1 (a) shows the schematic of thespecimen used in this study. Rebar with diameter of 10 mm was embedded in the cylindrical concrete with the size of 400 mm lengthand 50 mm diameter. Pull-out loading wasapplied to the rebar, and the strain distribution was measured along the rebar by 1
mm pitch. Figure 1 (b) shows the strain
distributions in the rebar in the reinforced
concrete measured using neutron diﬀraction
technique. Applied stress was gradually decreased from 200 MPa to 150 MPa during
strain measurement due to creep of the concrete. The strain distribution under the applied stress of 200 MPa was decreased in thelength from X=0 mm to 75 mm. Therefore,
it can be said that the length of the anchorage zone measured by neutron diﬀraction was
about 75 mm. Strain distribution measured
by strain gauges was also plotted in this ﬁgure. Decrease in the strain was observed in
the length from X=0 mm to approximately
225 mm, which means that the length of theanchorage zone measured by strain gauges
was approximately three times longer thanthat measured using the neutron diﬀraction
technique. Strain measurement using strain
原子炉：JRR-3

装置：RESA(T2-1)

gauge was probably aﬀected by the degradation of the boundary between concrete and rebar due to various treatments around strain
gauges. Therefore, it was conﬁrmed that theneutron diﬀraction technique, which is nondestructive and noncontact method, is useful technique for evaluating bond condition
between concrete and rebar accurately. Application of the neutron diﬀraction techniqueto the structural engineering ﬁeld will bringnew knowledge regarding design of the concrete structure.

Figure 1: (a) Schematic of the sample used in thisstudy and (b) comparison of strain distributions in therebar measured using neutron diﬀraction and strain
gauge.

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JAEA-Review 2013-039

1-10-4
Relaxation of Residual Stress in Engineering Component
K. Akita
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Compressive residual stress can enhance
the strength for fatigue and stress corrosion
cracking of engineering components and it canbe introduced on the surface layer by peening technologies such as shot peening andlaser peening. The compressive residual stressmight be relaxed due to the external mechanical load in service use. To clarify the initialresidual stress distribution is important to estimate the relaxation behavior because it superimposes on the external load.
In this study, the initial residual stress distribution was measured on a laser peened
sample using neutron diﬀraction. The material used in this study was an aluminum alloy, A2024-T3. The thickness of the sample
was 5 mm. Laser peening was applied on thesurface and back surface of the sample. Al311 diﬀraction was measured using RESA-II
in JRR-3. Lattice strains were obtained fromthe peak shift of the diﬀraction proﬁle. The
direction of the measured strain was parallelto the surface.

ual strain in the laser peened sample. Compressive strain induced by laser peening wasobserved in the surface layer. It decreased andchanged into tension at the depth of about
1.2 mm and reached to the maximum tension
at the center of the sample. Although theaccurate value of the residual stress should
be calculated from strains of three directions,the maximum tensile residual stress was estimated from the strain to be about 112MPa
under the assumption of equibiaxial planestress state. It was close to the value analyzed by a ﬁnite element method. The tensile
residual stress region will be deformed plastically at ﬁrst while the external tensile loadincreases. In this study, the existence of thetensile residual stress in the peened sample
was conﬁrmed. Relaxation behavior of theresidual stress in the external loading will bemeasured in the next experiment.

Fig. 1 shows the depth distribution of resid-

Figure 1: Depth distribution of residual in-plane strain on laser peened sample.

原子炉：JRR-3

装置：RESA-2(T2-3-2)

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JAEA-Review 2013-039

1-10-5Residual Stress Measurement of Thick Butt Weld
Using Neutron Diﬀraction
H. Suzuki, J. Katsuyama1 and Y. Morii
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
1
Safety Research Center, JAEA, Tokai, Ibaraki 319-1195

Accuracy of a neutron stress measurement
near the weldment is aﬀected by changes in
microstructure in a weld zone caused by phasetransformations, plastic strain generation andcrystal grain growth due to heating and cooling process during welding. Therefore, suitable diﬀraction planes, which are not aﬀectedby the plastic strains, and accurate stress-freelattice constant with consideration of changes
in microstructure should be ﬁgured out in order to measure accurate residual stress distribution near the weldment. In this study, it
was conﬁrmed that measuring lattice constantin stress-free condition using a standard sample makes it possible to select suitable reﬂections which are not aﬀected by the intergranular strains. Speciﬁcally, it can be determinedthat reﬂections of which lattice constants inthree orthogonal directions agree well with average lattice constant of all measured reﬂections are suitable.
This method was applied to residual stressmeasurements of 35 mm thick butt weld. It
was conﬁrmed that inﬂuence of intergranularstrain was negligible on the 311 and 220 reﬂections in austenitic steel and on the 110, 200
and 211 reﬂections in ferritic steel. Figure 1
shows results of residual stress distributions intransverse path in the center of wall thicknessof the 304SS butt weld and the 304SS-low alloy steel (A533B) dissimilar butt weld whichwere measured using 311 reﬂection in austenite and 211 reﬂection in ferrite. It was conﬁrmed that the residual stress distribution of
the 304SS butt weld was typical trend agreed
well with the stress distributions calculatedby the numerical simulations reported in previous studies, and that the residual stress distribution of the dissimilar weld was diﬀerent
from that of the 304SS butt weld since the dissimilar weld was aﬀected by the misﬁt of ther原子炉：JRR-3

装置：RESA(T2-1)

mal expansion coeﬃcient between austenitic
steel and ferritic steel.
This research project has been conductedunder the research contract with the Japan
Nuclear Energy Safety Organization (JNES).

Figure 1: Residual stress distributions in transverse
path in the center of wall thickness of the 304SS butt
weld (a) and the 304SS-low alloy steel dissimilar butt
weld (b).

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JAEA-Review 2013-039

1-10-6Development of Cryogenic Load Frame for Neutron Diﬀraction
H. Suzuki, Y. Tsuchiya1 , T. Umeno2 , S. Machiya3 and K. Osamura4
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
1
Quantum Beam Center, NIMS, Tsukuba, Ibaraki 305-0047
2
Taiyo Nippon Sanso Corporation, Tsukuba, Ibaraki 306-2611
3
Department of Mechanical Engineering, Daido University, Nagoya, Aichi 457-8530
4Research Institute for Applied Sciences, Kyoto 606-8202

In the cryogenic engineering ﬁeld, it isimportant to know material characterizationof engineering materials at low temperature.
Especially, evaluations of residual strains aswell as deformation behavior at low temperature are required for improving the strengthand the functionality of the cryogenic materials. For example, strain evaluations of engineered composite superconductors in service
are important to obtain higher performanceof superconductivity since that is aﬀected bystrains generated during fabrication process
and under operation. In order to achieve insitu strain measurement under loading at low
temperature, we have developed a cryogenic
load frame for neutron diﬀraction as shownin Fig. 1 (a). The load capacity of the load
frame was 10 kN and the lowest temperatureachieved at grips was below 4.8 K by using a
GM refrigerator. Figures 1 (b) and (c) show
the deformation behaviors of 111, 200 and
220 reﬂections of type 316 austenitic stainlesssteel under uniaxial tensile loading at room
temperature and 5 K. Linear response was observed in each diﬀraction at each temperatureand this result shows typical relation of whichrate of strain change at 5 K were smaller thanthat at room temperature.
This novel cryogenic load frame shows highest performance compared with similar instruments 1) prepared in the overseas engineering neutron facilities.
References
1) E. Oliver, B. Evans, M. Chowdhury, R. Major, O.
Kirichek and Z. Bowden : “Novel testing chamber
for neutron scattering in engineering materials at
cryogenic temperatures”, Meas. Sci. Technol., 19,034019(2008).

原子炉：JRR-3

装置：RESA(T2-1)

Figure 1: Overview of the developed cryogenic tensile
frame (a) and strain changes of three diﬀractions of an
austenitic type 316 stainless steel at room temperature(b) and approximately 5 K (c).

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JAEA-Review 2013-039

1-10-7Development of Multi-channel Vertical Conversing Slit
H. Suzuki, Y. Shinohara1 , T. Oku1 , J. Suzuki1 and M. Hayashi2
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
1
J-PARC Center, JAEA, Tokai, Ibaraki 319-1195
2
Ibaraki Prefectural Government, Tokai, Ibaraki 319-1106

Neutron stress measurement is very useful
to measure residual stresses in large scaled
mechanical components such as automobile
engines, large scaled welded tubes and so on.
In conventional optical system of the RESA
engineering diﬀractometer, the incident neutron beam size has been determined by a cadmium slit. In this case, the cadmium slit
should be installed at a position away fromthe sample to prevent the large scaled sample from bumping the slit during the measurement. Therefore, it was diﬃcult to make thebeam size ﬁne at the sample position, because
the divergent beam produced by the verticallyfocusing monochromator transmitts the cadmium slit and reaches the sample. In thisstudy, the multi-channel vertical conversing
slit (called “vertical radial collimator”) shownin Fig. 1(a) was developed to obtain the expected beam size with high ﬂux at sample position.
Figure 1(b) shows a simple schematic of
the optical layout of the RESA diﬀractometer with the vertical radial collimator. We
designed it to obtain 5mm of full width half
maximum (HF W HM ) of the incident beamheight at the sample position. Optimum
speciﬁcation of the vertical radial collimator
shown below was decided by the MacStas simulation.
*L1 (Conversing distance) = 500 mm*L2 (Length of collimator) = 384 mm*Number of channel = 10 ch
Figure 1(c) shows incident beam proﬁlesalong the vertical direction measured by aneutron imaging plate (NIP) at ﬁve positions of L1=410 mm, 455 mm, 500 mm, 545
mm and 590 mm. It was conﬁrmed thatthe beam intensity increased with approaching L1 to the designed value of 500 mm.
HF W HM at L1=500 mm was approximately
原子炉：JRR-3

装置：RESA(T2-1)

5.0 mm, showing good agreement with the
expected width. The incident beam proﬁleand integrated intensity (Iint in Fig. 1(c)) at
L1=500mm were almost the same as those at
L1=100mm when using a cadmium incident
slit. This result indicates that the neutron
beam diﬀracted from all silicon crystals of
monochromator system could eﬀectively converge on the sample position by using the vertical radial collimator.

Figure 1: (a) Overview of the vertical radial collimator
installed at the RESA diﬀractometer, (b) schematicof optical system of the RESA diﬀractometer with thevertical radial collimator and (c) incident beam proﬁles along the vertical direction by a neutron imaging
plate (NIP).

分野：中性子散乱（残留応力）- 291 -

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JAEA-Review 2013-039

1-11-1
Anomalous Lattice Dynamics in Relaxor K1−x Lix TaO3
S. Wakimoto, H. Taniguchi1 , G. A. Samara2 , R. K. Grubbs2 , E. L. Venturini2 , L. A. Boatner3
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Materials and Structure Laboratory, Tokyo Institute of Technology, Yokohama 226-8503
2
Sandia National Laboratories, Albuquerque, New Mexico 87185, USA
3
Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA

Relaxor K1−x Lix TaO3 shows rich dielectric properties with doping. Undoped compound KTaO3 is a quantum paraelectric material which never undergoes a ferroelectric(FE) transition, 1) in spite of the softened
FE phonon mode. 2) Li-doped system shows
relaxor behavior at high temperatures and
FE transition at low temperature. This happens because the doped Li+ ion occupies oﬀcentered position due to the small ionic radius, resulting in a large dipole moment anda precursor to the polar nano-region. Therefore, the dynamics of the doped Li ions areimportant to understand the relaxor behavior.
So far, there is no conclusive observation of
the Li dynamics. Only Raman scattering reported an anomalous mode appears only inthe doped samples and only in the relaxor
state. 3) These data are summarized in Fig.
1 by open symbols. This mode, here we referas ”impurity mode”, softens with decreasing
temperature following a universal line. However Raman data is restricted to the zone center (ZC) information. We have performed
inelastic neutron scattering to investigate qdependence of this impurity mode.
Crystals with x = 0.05 and 0.10 for thisstudy were grown by the slow-cooling method.
The neutron inelastic scattering measurements were done at the TAS-2 with ﬁxed ﬁnal
neutron energy at Ef = 14.7 meV and collimation sets of Guide(15 )-80-80-open. The
impurity mode has very weak intensity and,furthermore, it locates at the energy close to
the strong acoustic phonon. Thus the measurements near the zone center were unsuccessful. However, we succeeded to observe
the impurity mode near the zone boundary ofM-point, such as (1.5, 0.5, 0) and (1.5, 1.5, 0),
原子炉：JRR-3

装置：TAS-2(T2-4)

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4.

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Energy (cm-1)

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Temperature (K)Figure 1: Temperature dependence of the impurity
energy mode for various dopings. Open symbols indicate data from Raman scattering, that is the impurity mode energy at the zone center. Closed circles
show neutron data measured at the zone boundary(M-point).

where the acoustic phonon goes to well higher
energy (ω ≥ 12 meV). The observed impurity mode energies for both samples are shownin Fig. 1 by closed symbols. The impurity
mode energies at ZC (Raman data) and M
points (neutron) agree at higher temperatures(≥ 200 K). It is remarkable that only ZC energy softens with decreasing temperature implying that the impurity mode becomes dispersive at low temperatures. This behavior
can be understood that the Li ion dynamics is
uncorrelated with each other at high temperature where the relaxor behavior is dominant.
As temperature decreases they correlate eachother resulting in a ferroelectric transition.
References
1) S. H. Wemple, Phys, Rev. 137, A1575 (1964).
2) J. D. Axe, J. Harada, and G. Shirane, Phys. Rev.
B 1, 1277 (1970).
3) R. L. Prater, L. L. Chase, and L. A. Boatner,
Phys. Rev. B 23, 5904 (1981).

分野：中性子散乱（その他）- 295 -

JAEA-Review 2013-039

1-11-2

Neutron diﬀraction experiments of valence ﬂuctuating YbPd
A. Mitsuda A , M. Sugishima A , K. OhoyamaB , H. Wada A
A Dept. of Phys., Kyushu Univ., B IMR, Tohoku Univ.

30000

Intensity (Counts/30min)

Figure 1 shows the results of the experiments measured at 0.72 K and 3.62 K. The
overall diffraction patterns at both temperatures can be indexed as the cubic CsCltype structure, suggesting absence of thestructural transition. At 0.72 K, however, ashallow shoulder is found at around 2θ =5◦ . Since there exists no shoulder in thepatterns at 3.62 K, the shoulder is a magnetic Bragg peak. The low angle of 2θ indicates a long-periodic, possibly incommensurate, magnetic structure. The magnetic
Bragg peak, which is obtained by subtracting the diffraction pattern at 3.62 K fromthat at 0.72 K, is small and not broadened,
which suggests shrinkage of the magnetic
moment and long-range magnetic order.
Analysis of structure of magnetic order andcharge order is now in progress.
References:[1] R. Pott et al., Phys. Rev. Lett. 54 (1985)
481.
[2] P. Bonville et al., Phys. Rev. Lett. 57(1986) 2733.

Intensity (Counts/30min)

The cubic CsCl-type compound YbPd isknown to be a valence ﬂuctuating compound and to undergo 4 phase transitions
at 0.5, 1.9, 105, and 125 K [1]. 170 Yb
Mössbauer studies reveal that the one at
TM = 1.9 K is due to magnetic order [2]. However, the mechanisms of theother three phase transitions remain unknown. The Mössbauer studies also suggest magnetic and nonmagnetic Yb ionscoexist in equal proportions at low temperatures [2]. Assuming that the difference in magnetism is ascribed to two Ybvalence states, of which are nonmagnetic
Yb2+ and magnetic Yb3+ , the two valence
states should arrange regularly at low temperatures to make entropy zero. Such behavior, which is called ’charge order’, is observed in Yb4 As3 , Fe3 O4 and so on. These
compounds have low carrier density, while
YbPd exhibits metallic behavior. We are interested in the charge order of the metallic compound. We take notice of the factthat magnetic order and charge order coexist below 1.9 K according to the Mössbauer
studies. If we can determine the spin structure, the structure should include information on structure of the charge order since
only Yb3+ ions have a magnetic moment.
Therefore, in the present study, we perform powder neutron diffraction experiments of YbPd at low temperatures to determine spin and charge structure.
The experiments were carried out at
IMR-HERMES powder diffractometer. A
powdered sample (about 3 grams) was
loaded in the vanadium cell with the diameter of 8.6 mm, and then attached to the
1 K refrigerator. The powder diffraction
patterns were taken at 0.72 K and 3.62 K,
which is below and above magnetic ordering temperature of 1.9 K. The measurements were carried out twice at the same
temperature.

YbPd
λ=1.8204Å

20000

6000
4000
2000
0

10000

+3000
+2000
+1000

5
10
15
2θ (degree)
T=3.62K(2nd)
T=3.62K(1st)
T=0.72K(2nd)
T=0.72K(1st)
+3k
+2k
+1k

0

50

100
2θ (degree)

150

Fig. 1. Neutron diffraction patterns of YbPd at 3.62
and 0.72 K. The inset exhibits an enlarged grapharound 2θ = 5◦ . The arrows show a magnetic Bragg
peak.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 708- 296 -

JAEA-Review 2013-039

1-11-3Structural Evaluation of Titanate Nanotube and Nanosheet
A. Nakahira1, T. Kubo1 and M. Yashima2
Osaka Prefecture University1 and Tokyo Institute of Technilogy2
Nanomaterials with one-dimensional
nanostructures have attracted much attention due to their potential applications
in a variety of novel devices. Especially,
TiO2-derived nanotubes which are prepared by a hydrothermal treatment ofTiO2 particles in a concentrated NaOH
aqueous solution are expected to be usefulfor several application studies on suchas proton conduction, photoinducedhydrophilicity, photocatalysts,and dyesensitizing solar batteries. However, thecrystalline structure and formation mechanism of TiO2-derived nanotubes are still
topics under discussion. The elucidationof the crystalline structure and formation
mechanism for TiO2-derived nanotubes
will be expected to lead to the further
development of novel functional materials
with one-dimensional nanostructures. The
structural change on the molecular scaleof anatase-type TiO2 during a hydrothermal treatment was investigated in detailby various analytic techniques such as
neutron diffraction in order to clarify theformation mechanisms of titanate based
nanotubes.
Two grams of anatase-type TiO2 powder
as a starting material were used. They wereadded in 10 M NaOH aqueous solution.
Then the specimens were treated under thehydrothermal reaction at 383 K for 1 to 96
h. Obtained products after hydrothermal
treatments were sufﬁciently washed with
deuterated water and dilute HCl aqueous
solution and were subsequently separated
from the washing solution by ﬁltration. After the washing treatment, they were ﬁltered and subsequently dried at temperatures above 323 K for more than 12 hin an electric oven. Structural evaluationof titanate nanotube samples were evaluated by neutron diffraction at HEMES station. The neutron powder diffraction ex-

periments were conducted for room temperature using the HERMES powder neutron diffractometer installed on Tl-3 portof JRR-3M reactor in the Japan Atomic
Energy Research Institute (JAERI), Tokai,
Japan. An incident neutron wavelength λ= 1.8196 Å was obtained from a Ge (311)monochromator. The ND data were collected on thoroughly ground powders by amultiscanning mode in the 2 θ range from
5 °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×30 mm).
Fig.1(A) shows the typical structure image of nanotube products prepared by thehydrothermal process. The neutron diffraction pattern shows that the spectrum wasunsufﬁcient for the analysis because of theunsifﬁcient substitution of deuterated water in the nanotube structure, as shown in
Fig.1(B). It was hard to analysis because
there were high backgrounds in the observed data. This is thought to be why thepresence of a slight amount of H (H2O)
in the measuring sample. For this result,it was found that it was very difﬁcult toprepare a specimen of TiO2-derived nanotubes for ND measurements by using soft
However, it revealedchemical process.
that the nanosheet-like products composedof highly distorted TiO6 octahedra weregenerated by a hydrothermal treatment of
anatase-type TiO2 and then the anataselike structures are partially built up withthe formative nanotubes by scrolling up
these nanosheet-like products.

Activity Report on Neutron Scattering Research: Experimental Reports 16 (2009)
Report Number: 969- 297 -

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JAEA-Review 2013-039

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2.  ୰ ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕ 

2. Neutron Radiography- 299 -

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JAEA-Review 2013-039

2-1
Development of the Very High-Frame-Rate and High Resolution
Neutron Radiography System for High Speed Multi-Phase Flow
Visualizations
M. Kureta
Nuclear Science and Engineering Directorate, JAEA, Tokai, Ibaraki 319-1195

A high-frame-rate neutron radiography system [1] was remodeling in order to keep up
to the very high speed multi-phase ﬂow phenomena. The main point of the remodeling was the image intensiﬁer (I.I.). Luminas
gain and resolution were increased. The neworder-made I.I. system was consisted from two
types of the large size and high gain photoelectric multiplayer, one MCP and one imaging buster, with the special relay lens. Resolution could be 1024x1024 pixels when we used
the high speed camera (Photron FastcamP01BW). Brightness of the image could becontrolled by the gain of the MCP. In order
to conﬁrm the applicability of the new system
to the very high speed phenomena, fundamental test was carried out at the TNRF in the
research reactor JRR-3 of JAEA. Sample wasvery simple bubbling water which was ﬁlled in
the aluminum can. In the sample, air bubbles
were generated by the small pump with a sandstone. Figure 1 shows the instantiates imageof the test result. Recording speed of Figure
1 (a) and (b) were 2,000 fps and 6,000 fps,
respectively. It was conﬁrmed from the fundamental test that the new system was useful for the very high speed phenomena with
6,000 fps (512x512 pixels) or for high resolu-

Figure 1: Sample image((a)2,000fps,(b)6,000fps)

tion with 1,024 x1,1024 pixels (2,000fps). The
new system was applied to the visualization
test of the car engine as shown in Figure 2.
The test was carried out with NISSAN experimental group who prepared the experimental car engine. The purpose of the test was
to make clear the oil phenomena under theworking condition. The new imaging system
could be used for the high speed driving modeof the car engine.

References
1) M. Kureta et al. :“Jpn. J. Multi-Phase Flow.”,
Vol.23[2], pp. 165-173 (2009).

Figure 2: Application of the new system

原子炉：JRR-3

装置：TNRF(7R)

分野：中性子ラジオグラフィー（熱水力）- 301 -

JAEA-Review 2013-039

2-2
Development of Multi-pinhole Collimator for Large Imaging Area with Highspatial Resolution
H. Hayashida, M. Segawa, R. Yasuda, H. Iikura, T. Sakai, M. Matsubayashi
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

There are two kinds of factors aﬀecting tospatial resolution in radiography; one is theresolution of detector system and the other isthe beam optimization. In this study, topic is
focused to beam optimization.
A multi-pinhole collimator system which is
eﬀective for retaining imaging area with highspatial resolution has been demonstrated on
Cold Neutron Radiography Facility (CNRF)
at JRR-3M in JAEA. The multi-pinhole collimator system consists of a multi-pinhole aperture and an overlap-cutter (Fig. 1). On neutron beam from multi-pinhole aperture, neutrons from each pinholes make overlap at sample position due to beam divergence. In theoverlap area, sample images become split images. The overlap-cutter works to cut neutrons contribute to overlap at sample positionand enable us to get image without split.
In this study, a demonstration was performed with three conditions as written below, (a), (b) and (c), in order to verify
the eﬀect of multi-pinhole collimator system. A plastic model mainly fabricated bypolystyrene was used as a sample (Fig. 2) andan imaging plate (IP) was used as a detector
with resolution of 50 μm(a) Using large single pinhole
A large size aperture with a size of 35 mm
in vertical and 17mm in horizontal was used.
The distance between the aperture and sample L was 900 mm and the distance between
the sample and detector l was 100 mm. In thiscondition, unsharpness of image d, a parameter of spatial resolution, is not deﬁned by L/Dbut by beam divergence of 14 mrad. Thus dis estimated to 1.4 mm. The result is shownin Fig. 3(a). The size of the imaging area isabout 50 mm × 50 mm which corresponds tothe square area shown in Fig. 2.
(b) Using multi-pinhole aperture(without
overlap-cutter)

The multi-pinhole aperture was set andthe overlap-cutter was not used. The multipinhole aperture had 6 pinholes with each diameter of 2 mm and the distances of each pinhole were 10 mm as shown in Fig. 1(a). A geometrical setup was same with the condition(a), the distance between the multi-pinhole
aperture and sample L = 900 mm and l = 100
mm. In this condition, d is estimated to 0.22
mm by L/D = 450. The result is shown in
Fig. 3(b). An imaging area is about 50 mm
× 50 mm which is same with the condition(a) and clear image is obtained. This resultshows that using multi-pinhole aperture is effective to ratain imaging area with high spatial resolution. However, neutron beam which
contributes to overlap at sample position exists and split image is observed signiﬁcantly
in cheek parts of sample indicated by arrows
in Fig. 3(b).

原子炉：JRR-3

分野：中性子ラジオグラフィー（その他）

装置：CNRF(C2-3-3-1)(c) Using multi-pinhole collimator system
The multi-pinhole collimator system using
both of multi-pinhole aperture and overlapcutter was set. The distance between themulti-pinhole aperture and sample L = 900
mm and l = 100 mm. The overlap-cutter was
set at 255 mm downstream of multi-pinhole
aperture. A picture of overlap-cutter is shownin Fig. 1(b). Neutron beam which contributes
to overlap from pinhole (1) and (2) in Fig.
1(a) is cut by (4) part on overlap-cutter shownin Fig. 1(b) and from pinhole (1) and (3) is
cut by (5) part, similarly. All the neutron
beam contributes to overlap from each pinhole are cut by overlap-cutter in the sameway. Since the overlap-cutter works only to
cut neutrons contribute to overlap, unsharpness d is same with condition (b) and d isestimated to 0.22 mm. The result is shownin Fig. 3(c). Clear image is obtained without
split and an imaging area is about 50 mm ×
50 mm.

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JAEA-Review 2013-039

Three stripes indicated by arrows shown in
Fig. 3(c) are observed. A shape of the stripe
is same shape with the overlap-cutter and thestripe can be treated as image of the overlapcutter. When we have to get image in thisregion, we have to change a sample position.
The test experiment using the multipinhole collimator system was performed at
CNRF. Although we have to scan the sample position in order to get images on stripe
parts shown in Fig. 3(c), the system is effective to get a wide and clear image without sprit even in compact radiography instrument. In this demonstration, unsharpness d
is improved from 1.4 mm to 0.22 mm with asame imaging area of 50 mm × 50 mm. In thesystem, since the multi-pinhole aperture andthe overlap-cutter can be changed easily, it ispossible to install another radiography instrument. Furthermore we can control unsharpness d by changing each pinhole diameters.

Figure 2: The photograph of a sample.

Figure 1: (a) and (b) are the picture of multi-pinhole
aperture and overlap-cutter, respectively.

Figure 3: (a), (b) and (c) are the results from experimental conditions of (a), (b), and (c), respectively.

2-2- 303 -

JAEA-Review 2013-039

2-3
Evaluation of Spatial Resolution in Computed Tomography Images used Single
Aperture Devices in Thermal Neutron Radiography Facility in JRR-3
H. Iikura, R. Yasuda, H. Hayashida, T. Sakai and M. Matsubayashi
Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195

Recently, single aperture devices were installed in Thermal Neutron Radiography Facility (TNRF) in JRR-3. Then we evaluatedthe spatial resolution of computed tomography (CT) images with the devices. In thisstudy, size of aperture we used was 5.1 mm,
and L/D with the aperture device was 460
as against 176 without that. In addition, weused not only a standard NE426 scintillator,
but also the thinner ZnS:Ag/6 LiF scintillator
developed by JAEA.
Neutron image was taken through a cooled
CCD(Charge-Coupled Device) camera. At
ﬁrst, we used gold wires of ﬁve kinds of diameters on an aluminum stick (Fig. 1a). Without the single aperture device, the gold wire
was recognized to 200 μm, but the wire of
100 μm was not detected (Fig. 1b). But thegold wire of 100 μm was detected clearly with
5.1 mm aperture and the thinner scintillator(Fig. 1c, arrow). Next, we used gold wires ofthree kinds of diameters in an aluminum stickin various intervals. CT images were shownby Fig. 2(a) and (b) using pseudo color withand without 5.1 mm aperture and the thinner scintillator. Figure 2(c) shows comparison of spatial proﬁles in each CT image. With
the aperture device and the thinner scintillator, the spatial resolution is improved 2 times
higher.

Figure 1: CT images of gold wires of various diameters
on an aluminum stick. (a): Conﬁguration of the gold
wires setting. (b): CT image of gold wires without single aperture device. (c): CT image of gold wires with
5.1 mm aperture and the thinner scintillator. Arrowshows a gold wire of 100 μm diameter.

Figure 2: CT images of gold wires which set in various
intervals in an aluminum stick. (a): CT image of gold
wires without single aperture device. (b): CT imageof gold wires with 5.1 mm aperture and the thinner
scintillator. (c): Comparison of spatial proﬁles in each
CT image.

原子炉：JRR-3

装置：TNRF(7R)

分野：中性子ラジオグラフィー（その他）- 304 -

JAEA-Review 2013-039

2-4Visualization of Water Behavior in an Operating Fuel Cell
H. Iikura, R. Yasuda, T. Sakai, M. Matsubayashi and Y. Katada1
1

Quantum Beam Science Directorate, JAEA, Tokai, Ibaraki 319-1195
Fuel Cell Materials Center, National Institute for Materials Science, Tsukuba, Ibaraki 305-0047

As a collaborative research with National
Institute for Materials Science (NIMS), we
conducted visualization of water behavior inan operating polymer electrolyte fuel cell
(PEFC) using the JRR-3 thermal neutron
radiography facility (TNRF). The PEFC iscompliant with a Japan Automobile ResearchInstitute (JARI) standard PEFC. On a JARI
standard PEFC, an active area is 50 x 50 mm2
and a ﬂow channel for H2 and air gases is single parallel serpentine; the width, depth andpitch of which are 1 mm, each. For optimizing the PEFC for neutron imaging, clamping
plates (original: stainless steel) were replacedwith those of aluminum. Also, for the purposeof experiment, separator plates (original: carbon) were replaced with those of aluminum orhigh nitrogen steel (HNS).
NIMS is developing high corrosion resistantseparator materials, such as HNS. To conﬁrm availability of HNS as separator materials of a PEFC, we started to compare theperformance of HNS with those of carbon,
aluminum and so on. Thermal neutron transmittance of a 6 mm thick HNS separator plate
was worse than that of an original 10 mmthick carbon separator plate. However, we
conﬁrmed that the subtraction image showedexistence of water in a ﬂow channel of HNS
separator clearly.
Real-time neutron imaging system using an EB(Electron Bombard)-CCD(ChargeCoupled Device) camera with frame rate of
30 frames/s coupled with an NE426 equivalent ﬂuorescent converter (NR converter, Kasei Optonix) was used. Captured neutron
images were recorded on a hard disk video
recorder as NTSC (National Television System Committee) format. A fuel cell operating system which was prepared by NIMS, wasinstalled at the TNRF as shown in Fig. 1.
As a result of power generation of the
原子炉：JRR-3

装置：TNRF(7R)

PEFC, product water was not clearly observed by the real-time neutron imaging system, but condensed water behavior in ﬂow
channels of separator plates was clearly observed as shown in Fig. 2. The neutron imaging using an EB-CCD camera system is considered to be available for visualizing of water
behavior in ﬂow channels of 1 mm depth andwidth such as JARI standard PEFCs.

Figure 1: Photograph of an operating PEFC.

Figure 2: Neutron image of condensed water behavior
in PEFC using an EB-CCD camera (1 frame[1/30s]).

分野：中性子ラジオグラフィー（その他）- 305 -

JAEA-Review 2013-039

2-5
඲ᅛయ஧ḟ㟁ụ࡟࠾ࡅࡿ㟁ᴟ࣭㟁ゎ㉁୰ࡢ
Ỉ⣲࡞ࡽࡧ࡟ࣜࢳ࣒࢘ࡢศᕸ࣭ᣑᩓ≧ែࡢゎ᫂Investigation of Distribution and Diffusion of Hydrogen and Lithium in the Electrode andElectrolyte Materials for All-Solid State Rechargeable Batteries◊✲௦⾲⪅ 㫽ྲྀ኱Ꮫ኱Ꮫ㝔 ᆏཱྀ⿱ᶞ㻌◊✲༠ຊ⪅㻌 㫽ྲྀ኱Ꮫ኱Ꮫ㝔㻌 Ụᆏா⏨䠈༡᮲┿బே䠈㧗஭ⱱ⮧䠈㣤⏣㈗ஂ㻌㻶㻭㻱㻭㻌 ᯇᯘᨻோ䠈㣤಴ᐶ㻌䝷䝣䜱䞊(NR)䜢⏝䛔䛶ほ㸦㸯㸧 ࡣ ࡌ ࡵ ࡟⌧ᅾ䝸䝏䜴䝮䠎ḟ㟁ụ䛿ᦠᖏ➃ᮎ䜔⮬ື㌴⏝㟁※䛻䛧䛶䛝䛯䠊䛣䜜䜎䛷䛿䠈ி኱

ཎᏊ⅔ᐇ㦂ᡤ䛷ᅛయ㟁ゎ㉁(Li4/3Ti5/3O4 䠈LISICON䠈௦⾲䛥䜜䜛䜘䛖䛻䠈ᡃ䚻䛾⏕ά䛻Ḟ䛟䜉䛛䜙䛦䜛䝕䝞䜲

La2/3-xLi3xTiO3)䜢୰ᚰ䛻䝖䝺䞊䝃䞊ᣑᩓಀᩘ䜢䝇䛸䛺䛳䛶䛚䜚䠈䛥䜎䛦䜎䛺ほⅬ䛛䜙⢭ຊⓗ䛻◊✲䛜⾜䛝䛯䛜䠈ᖹᡂ 18 ᖺᗘ䛛䜙୰ᛶᏊ䝡䞊䝮䛾ᥦ౪䜢ఇṆ䛧䜟䜜䛶䛔䜛䠊⌧ᅾ䛾䠎ḟ㟁ụ䛾ᶆ‽ⓗ䛺ᵓᡂ䛿䠈㈇ᴟ

䛶䛔䜛䛯䜑䠈ᐇ㦂᪋タ䜢ཎ◊ JRR-3M ෭୰ᛶᏊ䝫䞊䝖(C)/᭷ᶵ㟁ゎᾮ/ṇᴟ (LiCoO2 䜔 LiMn2O4䠈LiFePO4 䛺䛻⛣䛧䠈ྠᵝ䛾ᡭἲ䛷䝸䝏䜴䝮ṇᴟᮦᩱ䛻ᑐ䛧䛶䝖䝺䞊䛹)䛷䛒䜛䛜䠈Ᏻ඲㠃䜔ྲྀ䜚ᢅ䛔䛾⠊ᅖ䛾ᣑᙇ䛸䛔䛳䛯䝃䞊ᣑᩓᐇ㦂䜢㛤ጞ䛧䛯䠊NR 䛷ྠ఩య⃰ᗘศᕸ䜢

Ⅼ䛛䜙䠈㟁ゎᾮ䜢ᅛయ㟁ゎ㉁䛸䛧䛯඲ᅛయ஧ḟ㟁ụ䛜ᐃ䛧䛶䝖䝺䞊䝃䞊ᣑᩓಀᩘ䜢ồ䜑䜛ᮏᡭἲ䛿䠈௚䛾᪉䛥䛛䜣䛻◊✲䛥䜜䛶䛔䜛䠊䛣䛾ሙྜ䠈ᅛయ㟁ゎ㉁䛾䜲䜸

ἲ䛻ẚ䜉䛶ᴟ䜑䛶☜ᗘ䛾㧗䛔ᣑᩓಀᩘ䞁ఏᑟ⋡䜔㟁ᴟ/㟁ゎ㉁⏺㠃䛷䛾཯ᛂ䛜Ỵᐃⓗ䛺䝟䝷䛒䜚䠈䜎䛯໬Ꮫᣑᩓಀᩘ䛷䛿䛺䛟䝖䝺䞊䝃䞊ᣑᩓಀᩘ䛜䝯䞊䝍䛻䛺䜛䛾䛿䜒䛱䜝䜣䛾䛣䛸䠈ṇᴟෆ㒊䜎䛷ධ䜚㎸䜣ᚓ䜙䜜䜛䛸䛔䛖≉ᚩ䜢䜒䛴䠊

ᐃ䛧䛶

ᐃ䛜ྍ⬟䛷

䛷䛔䛯䛷䛒䜝䛖㟁ゎᾮ䛜ᅛయ䛻䛺䜜䜀ṇᴟ⮬య䛾ᣑᩓ䝇䝢䝛䝹ᆺᵓ㐀䜢♧䛩 LiMn2O4 䛿䠈⌧ᅾᗈ䛟⏝䛔䜙ಀᩘ䛾⤯ᑐ್䜒㔜せ䛺䝟䝷䝯䞊䝍䛸䛺䜛䠊LiCoO2 䜔䜜 䛶 䛔 䜛 LiCoO2 䛾 䜘 䛖 䛻 ᕼ ᑡ 㔠 ᒓ 䜢 ྵ 䜎 䛪 䠈 䜎 䛯

LiMn2O4 䛺䛹䛾ṇᴟᮦᩱ䛿㟁Ꮚ䞉䜲䜸䞁ΰྜఏᑟయ䛷

LiFePO4 䛸ẚ䜉䛶䝸䝏䜴䝮ᣑᩓಀᩘ䛜㧗䛔䛸䛥䜜䛶䛔䜛䛒䜚䠈䛣䜜䜎䛷䛻ሗ࿌䛥䜜䛶䛔䜛䝸䝏䜴䝮䜲䜸䞁䛾ᣑᩓಀ䛣䛸䛛䜙䠈༢య䛸䛧䛶䜒䠈䛒䜛䛔䛿 Li(Co, Mn, Ni)O2 䛾䜘䛖ᩘ 䛿 䠈 GITT (Galvanostatic Intermittent Titration䛺ΰᬗ⣔䛸䛧䛶䜒᭷ᮃ䛺ṇᴟᮦᩱ䛷䛒䜛䠊䜎䛯䠈䝲䞊䞁Technique)䛺䛹䛾㟁Ẽ໬Ꮫⓗᡭἲ䛻䜘䛳䛶ᚓ䜙䜜䛯䜒䝔䝷䞊ṍ䜏䛜ᐜ㔞పୗ䜢ᘬ䛝㉳䛣䛩䛣䛸䠈඘㟁㏵୰䛾䛾䛷䛒䜛䠊䛣䛾ᡭἲ䛷䛿㟁ᴟ䛻䛚䛡䜛㟁Ⲵ䛾ฟධ䜚(䛸(Li 䛾ᑡ䛺䛔)ヨᩱ䛷䛿 Li ✵Ꮝ䛜ከ䛔䛻䜒䛛䛛䜟䜙䛪໬㟁ᅽ)䛾䜏䜢ほ䛧䛶䛔䜛䛯䜑䠈ู䛾཯ᛂ䜔⌮᝿ⓗ䛺䝰Ꮫᣑᩓಀᩘ䛜ప䛔䛺䛹䛾⌧㇟䜒▱䜙䜜䛶䛚䜚䠈㟁ụタ䝕䝹䛛䜙䛾䛪䜜䠈䛒䜛䛔䛿௚䛾䝟䝷䝯䞊䝍䛾ぢ✚䜒䜚䛻ィୖ䛾ᇶ♏䝕䞊䝍䛸䛧䛶䜀䛛䜚䛷䛺䛟䠈ᮦᩱ⛉Ꮫ䛾ほⅬ኱䛝䛟౫Ꮡ䛧䠈ሗ࿌䛥䜜䛶䛔䜛್䛻䜒䛛䛺䜚ᖜ䛜䛒䜛䠊䛛䜙䜒☜ᗘ䛾㧗䛔䝖䝺䞊䝃䞊ᣑᩓಀᩘ䛾ᡃ䚻䛾◊✲䜾䝹䞊䝥䛿䝸䝏䜴䝮䛾Ᏻᐃྠ఩య 6Li 䛸
7

7䜜䛶䛔䜛䠊ᮏሗ࿌䛷䛿䠈୰ᛶᏊ䝷䝆䜸䜾䝷䝣䜱䞊䛻䜘䜚Li 䛷୰ᛶᏊ䛾྾཰ಀᩘ䛜ᩘ᱆㐪䛖䛣䛸䜢฼⏝䛧䛶䠈 Li

LiMn2O4 䛾㧗䛛䜙䛺䜛ヨᩱ䛻 6Li 䛜ᣑᩓ䛩䜛ᣲື䜢䠈୰ᛶᏊ䝷䝆䜸䜾䜑䛯⤖ᯝ䛻䛴䛔䛶㏙䜉䜛䠊

JRR-3Mᐃ䛿ษᮃ䛥㡿ᇦ䛻䛚䛡䜛䝖䝺䞊䝃䞊ᣑᩓಀᩘ䜢ồ

CNRF ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕࣮⿦⨨ ᮦᩱ໬Ꮫ㻝㻣㻟

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JAEA-Review 2013-039

㸦㸰㸧 ᐇ 㦂㸦㸱㸧 ⤖ᯝ࡜⪃ᐹ

7

㻌 ᣑᩓヨᩱ䛾 LiMn2O4 䛿㏻ᖖ䛾ᅛ┦཯ᛂἲ䛷ㄪ〇䛧㻌 㻲㼕㼓㻚㻌 㻝 䛻 㻸㼕㻹㼚㻞㻻㻠 䛾ᶆ‽ヨᩱ䛸ᣑᩓヨᩱ䛾୰ᛶᏊ䝷

䛯䠊 7Li2CO3 䛚䜘䜃 Mn2O3 䜢໬Ꮫ㔞ㄽẚ䛻ΰྜ䛧䠈䝆䜸䜾䝷䝣䜱䞊㻔㻺㻾㻕ീ䛸䛭䛾ᙉᗘ䝕䞊䝍䛾౛䜢♧䛩䠊ᕥ

600䉝䛚䜘䜃 800䉝䛷䛭䜜䛮䜜 10 ᫬㛫↝ᡂ䛧䛯䠊ᚓ䜙䛛䜙 㻝㻝 ಶ䛾ᶆ‽ヨᩱ䠈ᣑᩓヨᩱ䠈䛚䜘䜃ᣑᩓヨᩱྠ䛨䜜䛯ヨᩱ䛿 5 mm×5 mm×7 mm 䛾ゅᰕ≧䛻ᡂᙧ䛧䠈⢭䝃䜲䝈䛷 㻢㻸㼕 䜢ሬᕸ䛧䛶䛔䛺䛔ヨᩱ䜢୪䜉䛶 ᐃ䛧䛶䛔ᐦ䛻㛗䛥䜢ᥞ䛘䛯䠊䜎䛯䠈ྠ఩య⃰ᗘᰯṇ⏝䛻 6Li/7Li䜛䠊ᶆ‽ヨᩱ䛿 㻸㼕 䛜⮬↛ྠ఩యẚ䛾 㻺㻸㼕 䛛䜙 㻣㻸㼕 䜎䛷䛾ẚ䜢 10 %䛤䛸䛻ኚ໬䛥䛫䛯 LiMn2O4 䛻䛴䛔䛶䜒ྠᵝ㻝㻜㻑䛤䛸䛻ኚ໬䛥䛫䛶䛚䜚䠈㻢㻸㼕 ⃰ᗘ䛾㧗䛔ヨᩱ㻔㻺㻸㼕 ഃ㻕䛻ྜᡂ䛧䠈ྠ୍䛾ཌ䛥䛻ᡂᙧ䛧䛯䠊

䛷㏱㐣ᙉᗘ䛜ప䛟䛺䛳䛶䛔䜛䛣䛸䛜ほ㻌 ᣑᩓヨᩱ䛾∦㠃䛻 7LiNO3 㣬࿴⁐ᾮ䜢ᚤ㔞䛾㓑㓟䝉ᩱ䛿 㻢㻸㼕㻺㻻㻟 䜢ሬᕸᚋ 㻤㻜㻜㼛㻯 䛷 㻟 ᫬㛫䜰䝙䞊䝹䛧䛯䝹䝻䞊䝇䛸䛸䜒䛻ሬᕸ䛧䠈700䡚800䉝䛷ᣑᩓ䜰䝙䞊䝹䜢㻸㼕㻹㼚㻞㻻㻠 䛷䠈㻢㻸㼕 䜢ሬᕸ䛧䛯ヨᩱᕥ➃䛛䜙⃰䛔䜾䝷䝕䞊⾜䛳䛯䠊䜰䝙䞊䝹䛿 30 ศ䛤䛸䛻ఇṆ䛧䛶୰ᛶᏊ䝷䝆䜸䝅䝵䞁䛜ほ䜾䝷䝣䜱䞊 ᐃ䜢⾜䛔䠈ྠ୍ヨᩱ䛷䛥䜙䛻㛗᫬㛫䛾ᣑᩓ䜛䠊㻌䛥䜜䜛䠊ᣑᩓヨ䛥䜜䠈 㻢㻸㼕 䛜ᣑᩓ䛧䛶䜖䛟ᵝᏊ䛜ほ䛥䜜ᐇ㦂䜢⾜䛳䛯䠊䝷䝆䜸䜾䝷䝣䜱䞊ᐇ㦂䛿ཎ◊ JRR-3M ⅔

㻌 䛣䛾ᶆ‽ヨᩱ㒊ศ䛾 㻺㻾 䝕䞊䝍䜢⏝䛔䛶䠈㏱㐣ᙉᗘ䛸

CNRF 䝫䞊䝖䛷⾜䛳䛯䠊ᣑᩓヨᩱ䛸ྠ఩య⃰ᗘᰯṇ⏝㻺䛾ᶆ‽ヨᩱ䜢୍ิ䛻୪䜉䠈୰ᛶᏊ⏝䜲䝯䞊䝆䞁䜾䝥䝺⃰ᗘ䝥䝻䝣䜯䜲䝹䜢ồ䜑䜛䛸䠈㻲㼕㼓㻚㻌 㻞㻌 㻔㼍㻕䛜ᚓ䜙䜜䜛䠊䛥䜙

䞊䝖(NIP) 䜢䛭䛾⫼㠃䛻䝉䝑䝖䛧䛯䠊䛣䜜䜙䜢ヨᩱ䝩䝹䝎䛻ྠ఩య⃰ᗘ䛾ᑐᩘ䛸⾲㠃䛛䜙䛾㊥㞳䛾䠎஌䛾㛵ಀ䜢

-1㻸㼕 ⃰ᗘ䛾㛵ಀ䜢ồ䜑䠈䛣䜜䜢䜒䛸䛻ᣑᩓヨᩱ䛾ྠ఩య䞊䛻䝉䝑䝖䛧䠈୰ᛶᏊධᑕ᪉ྥ䛻ᆶ┤䛻 4 mms 䛾୍ᐃ䝥䝻䝑䝖䛩䜛䛸㻔㼎㻕䛾䜘䛖䛻䛺䜚䠈ഴ䛝䛿㻙㻝㻛㻠㻰㻖㼠 䜢୚䛘䜛䠊㏿ᗘ䛷䝇䜻䝱䞁䛩䜛䛣䛸䛻䜘䜚䠈IP 䛻↷ᑕ䛩䜛୰ᛶᏊ䛜㻣㻜㻜㻘㻌 㻣㻡㻜 䛚䜘䜃 㻤㻜㻜䉝䛷ᵝ䚻䛺᫬㛫䜰䝙䞊䝹䛧䛶ᚓ䜙㉮ᰝ᪉ྥ䛷ᆒ୍䛻䛺䜛䜘䛖䛻䛧䛯䠊䝷䝆䜸䜾䝷䝣䜱䞊䝕䜜䛯 㻺㻾 ീ䛛䜙ồ䜑䛯 㻰㻖㼠 䜢 㼠 䛻ᑐ䛧䛶䝥䝻䝑䝖䛧䛯ᅗ䛜䞊䝍䛿䜲䝯䞊䝆䝸䞊䝎䛷ㄞ䜏ฟ䛧䛯䠊㻲㼕㼓㻚㻌 㻟 䛷䛒䜛䠊䛔䛪䜜䜒䜘䛟┤⥺䛻㍕䜚䠈䜰䝙䞊䝹᫬㛫䛸

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Fig. 1

NR image and transmitted intensities of standard and diffusion samples of LiMn2O4.

JRR-3M

CNRF ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕࣮⿦⨨ ᮦᩱ໬Ꮫ

2-5
㻝㻣㻠

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JAEA-Review 2013-039

Fig. 2 (a) Isotope concentration profile of LiMn2O4 diffusion sample annealed at 800oC for 3 hours.
(b) ln(cN) – 'x2 relationship of the isotope concentration profile.
䛸䜒䛻ᣑᩓ䛜㐍⾜䛩䜛䛣䛸䛜䜟䛛䜛䠊䛣䛾ഴ䛝䛛䜙ồ䜑䛯㻌ᣑᩓಀᩘ䜢䜰䝺䝙䜴䝇ᆺ䛾䜾䝷䝣䛻䝥䝻䝑䝖䛩䜛䛸 㻲㼕㼓㻚㻌 㻠㻌䛜ᚓ䜙䜜䛯䠊㻌㻌㻌 ᮏ◊✲䛿 㻸㼕㻹㼚㻞㻻㻠 䛾䝖䝺䞊䝃䞊ᣑᩓಀᩘ䜢ồ䜑䛯᭱㻌ึ䛾◊✲䛷䛒䜛䠊௒ᅇ䛿 ᐃ䛧䜔䛩䛔 㻝㻜㻙㻤䡚㻝㻜㻙㻢㻌㼏㼙㻞㼟㻙㻝㻌⛬ᗘ䛾ᣑᩓಀᩘ䛻䛩䜛䛯䜑䛻䠈㻣㻜㻜䉝௨ୖ䛾㡿ᇦ䛷ᣑ㻌ᩓ䜰䝙䞊䝹䜢⾜䛳䛯䠊䛧䛛䛧௒ᅇ䛾䝕䞊䝍䛷䛿ᐃⅬ䜒㻌䛷⠊ᅖ䜒⊃䛔䛯䜑䠈䝸䝏䜴䝮㟁ụ䛾㏻ᖖ䛾౑

㻌

ᑡ䛺䛟㧗

⏝㡿ᇦ䛷䛒䜛ᐊ௜㏆䜎䛷ᣑᩓಀᩘ䛾್䜢እᤄ䛩䜛䛾䛿ᅔ㞴䛷䛒䜛䠊௒ᚋ䠈䜘䜚ప㻔䡚㻡㻜㻜䉝⛬ᗘ㻕䛾ᣑᩓヨᩱ䛷䛾 ᐃ䛜ᮃ䜎䜜䜛䠊㻌

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Fig. 4Arrhenius plots of tracer diffusion
coefficients for LiMn2O4.

2-5

Fig. 3 Annealing time dependence of D*tobtained from NR data.

JRR-3M

CNRF ୰ᛶᏊࣛࢪ࢜ࢢࣛࣇ࢕࣮⿦⨨ ᮦᩱ໬Ꮫ㻝㻣㻡

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3.  ᨺ ᑕ໬ศᯒ 

3. Neutron Activation Analyses- 309 -

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JAEA-Review 2013-039

3-1◊✲ࢸ࣮࣐㸸 40 Ar/ 39 Arᖺ௦ᐃ࡟ࡼࡿⅆᒣάືྐཬࡧᆅẆᵓ㐀Ⓨ㐩ྐࡢゎ᫂—᪥ᮏ࿘㎶ᾏᇦཬࡧάືⓗⅆᒣ࡟㛵ࡍࡿ◊✲—⾲   㢟㸸 40 Ar/ 39 Arᖺ௦ᐃ࡟ࡼࡿⅆᒣάືྐཬࡧᆅẆᵓ㐀Ⓨ㐩ྐࡢゎ᫂—᪥ᮏ࿘㎶ᾏᇦཬࡧάືⓗⅆᒣ࡟㛵ࡍࡿ◊✲—4 0 Ar/ 39 Arᖺ௦ᐃ࡟ࡼࡿⅆᒣάືྐཬࡧᆅẆᵓ㐀Ⓨ㐩ྐࡢゎ᫂—᪥ᮏ࿘㎶ᾏᇦཬࡧάືⓗⅆᒣ࡟㛵ࡍࡿ◊✲—▼ሯ἞ ࠊ ᯇ ᮏ ဴ ୍⏘ᴗᢏ⾡⥲ྜ◊✲ᡤ㸯㸬┠ⓗࣇ࢕ࣜࣆࣥᾏᾏᇦ࠾ࡼࡧࡑࡢ࿘㎶ࡢᑠ➟

Canyon Tuff (FC3)୰ࡢsanidineࢆ౑⏝ࡋࡓࠋᖺ ௦ ィ ⟬ ࡟ ࡣ ࠊ ࡇ ࡢ ᶆ ‽ヨ ᩱ ࡢ ᖺ ௦ ࡜ ࡋ ࡚ཎᾏྎࡸ༡㫽ᓥ࿘㎶ᾏᇦ࡟࠾࠸࡚㸪᥇ྲྀࡉࢀ

27.5Maࢆ⏝࠸ࡓ 1㸧 ࠋࡓ ᆅ ㉁ ヨ ᩱ ࡟ 㛵 ࡍ ࡿ ᆅ ⌫⛉ Ꮫ ⓗ ศ ᯒ ࢹ ࣮ ࢱࢦࣥྠ఩యࡢ⿵ṇࡣࠊK࡜Caࢆࡑࢀࡒࢀྵࡴ

≉࡟ᒾ▼ࡢᙧᡂᖺ௦ ࢆࡶ࡜࡟㸪ྛᾏᇦ࡟࠾

ྜᡂ࢞ࣛࢫࢆヨᩱ࡜࡜ࡶ࡟୰ᛶᏊ↷ᑕࡋࠊศࡅ ࡿ ࣐ ࢢ ࣐ ά ື ࠾ ࡼ ࡧ ࣐ࣥ ࢺ ࣝ ࢲ ࢖ ࢼ ࣑ ࢡᯒࡍࡿࡇ࡜࡟ࡼࡾ⾜ࡗࡓࠋヨᩱࡢ୰ᛶᏊ↷ᑕࢫ ➼ ࢆ ྵ ࡵ ࡓ ⅆ ᡂ ά ື ྐࢆ ᢕ ᥱ ࡍ ࡿ ࡇ ࡜ ࢆࡣࠊཎᏊຊᶵᵓᮾᾏ◊✲ᡤࡢJRR3 ࡟࡚ࠊHR2┠ⓗ࡜ࡍࡿ㸬ࡲࡓᮏ◊✲ࡣ⌧ᅾᅜ࡟ࡼࡾ‽ഛࢆ౑⏝ࡋ 24 ᫬㛫↷ᑕࢆ⾜ࡗࡓࠋࡲࡓ࢝ࢻ࣑ࡉ ࢀ ࡚ ࠸ ࡿ ᅜ 㐃 ࡬ ࡢ ᡃ ࡀᅜ ࡢ ኱ 㝣 Ჴ 㝈 ⏺ ⏬

࣒࢘⟩࡟ࡼࡿ⇕୰ᛶᏊ࢝ࢵࢺࢆ⾜ࡗࡓࠋᐃ⏦ㄳࡢࡓࡵࡢㄪᰝࡢ୍⎔࡛࠶ࡿࠋ᪥ᮏ࿘㎶ᐃࡢጉᐖ࡜࡞ࡿ࢔ࣝ ࢔ࣝࢦࣥࡢྠ఩యẚศᯒࡣࠊ⏘ᴗᢏ⾡⥲ᾏ ᇦ ࡢ ᇶ ┙ ᒾ ࡢ ⢭ ᐦ ࡞ ᙧᡂ ᖺ ௦ ࢆ Ỵ ᐃ ࡍ ࡿྜ ◊ ✲ ᡤ ࡢ ࣞ ࣮ ࢨ ຍ⇕ 40 Ar/ 39 Arᖺ ௦

ࡇ࡜ࢆ㏻ࡌ࡚ࠊᅜ㐃࡬ࡢᥦฟ᝟ሗసᡂࢆࢧ࣏

ࢫࢸ࣒࡟ࡼࡾ⾜ࡗࡓࠋศᯒἲ➼࡟ࡘ࠸࡚ࡣࠊ

࣮ࢺࡍࡿࠋ

2)

ᐃࢩ

ᐃࢩࢫࢸ࣒ࡣ 2007 ᖺᗘ࡟ᨵ࡟‽ࡌࡓࠋ㐀ࢆᐇ᪋ࠊ㸰㸮㸮㸶ᖺᗘ࠿ࡽᮏ᱁✌ാࡋࡓࠋ㸰㸬᪉ἲᐃ⏝ヨᩱ࡜ࡋ࡚ࠊⅆᒣᒾࡢ࠺ࡕࡶࡗ࡜ࡶ

᭱኱ࡢ㐪࠸ࡣࠊヨᩱຍ⇕࡟CO2 ࣮ࣞࢨࢆᑟධ

᪂㩭࡞▼ᇶ㒊ศࢆ୺࡟౑⏝ࡋࡓࠋヨᩱ࠿ࡽཌᐃ࡟ඛ❧ࡕࠊヨᩱࢆ┿✵୰࡟࡚⣙ 72 ᫬㛫ࡋࡓࡇ࡜ࠊࡉ⣙ 1mmࡢᯈ≧ヨᩱࢆษࡾฟࡋࠊࡑࢀࢆ㍍

ᐃࢆ᏶඲⮬ື໬ࡋࡓࡇ࡜࡛࠶ࡿࠋ

100 o C࡛↝ࡁࡔࡋࢆ⾜ࡗࡓࠋヨᩱࡢຍ⇕࡟ࡣࠊࡃ⢊○ࡋ࡚⣙ 1mmゅࡢᑠ∦࡟ࡋࡓࠋࡑࡢᚋ

CO2 ࣮ࣞࢨࢆ⏝࠸ࠊ࣮ࣞࢨࣅ࣮࣒ࡢᚄࡣヨᩱኚ ㉁ ࡟ ࡼ ࡾ ⏕ ࡌ ࡚ ࠸ ࡿ ྍ⬟ ᛶ ࡢ ࠶ ࡿ ⢓ ᅵ 㖔඲యࡀᆒ㉁࡟ຍ⇕ࡉࢀࡿࡼ࠺࡟⣙ 3.2mm࡜

≀ࡸⅣ㓟ሷ㖔≀ࡢ㝖ཤࢆ┠ⓗ࡜ࡋ࡚ࠊ3MHCl

ࡋࡓࠋヨᩱࡢ

୰࡛⣙ 30 ศࠊࡉࡽ࡟ 4MHNO 3 ୰࡛⣙ 30 ศᐃࡣẁ㝵ຍ⇕ἲ࡟ࡼࡾ⾜ࡗࡓࠋࢫࢸࢵࣉࡈ࡜࡟࣮ࣞࢨࡢฟຊࢆୖ᪼ࡉࡏࠊヨ㉸㡢ἼὙίᚋࠊ⬺࢖࢜ࣥỈ࡛ὙίࡋࡓࠋὙί

ᩱࡀ⼥ゎࢆ㛤ጞࡍࡿࡲ࡛ฟຊࢆୖ᪼ࡉࡏࡓࠋ

᫬㛫ࡣࠊヨᩱࡢኚ㉁⛬ᗘ࡟ࡼࡗ࡚ㄪᩚࡋࡓࠋ

ྛࢫࢸࢵࣉ࡛ࠊ࣮ࣞࢨࡢฟຊࢆ୍ᐃ࡜ࡋ࡚ࠊ

ὙίᚋỈ୰࡛⣙ 2 ᪥㛫⬺ሷฎ⌮ࢆ⾜ࡗࡓࠋ஝⇱ᚋࠊ㢧ᚤ㙾ୗ࡛ኚ㉁㒊ࡸᩬᬗࡢΰධࡢ࡞
࠸ヨᩱࢆࣁࣥࢻࣆࢵࢡࡋࠊ

90 ⛊㛫ຍ⇕ࡋࠊ ᐃࢆ⾜ࡗࡓࠋヨᩱ࠿ࡽᢳฟ
⢭ 〇 ࡉ ࢀ ࡓ ࢞ ࢫ ࡣ ࠊ 4 ಶ ࡢ Zr-Al ࢤ ࢵ ࢱ ࣮ᐃ⏝ヨᩱ࡜ࡋࡓࠋ

(SAES AP-10) ࡜ 1 ಶ ࡢ Zr-Fe-V ࢤ ࢵ ࢱ ࣮ ヨᩱࡣ࢔࣑ࣝ⟩࡟ໟࡳࠊᖺ௦ᶆ‽ヨᩱ

㸦SAES ST707㸧࡟ࡼࡾ 10 ศ㛫⢭〇ࡉࢀࡓࠋ㸦ࣇࣛࢵࢡࢫࣔࢽࢱ㸧࡜࡜ࡶ࡟ࠊ୰ᛶᏊ↷ᑕ⢭〇ᚋࠊVG Isotech♫㸦⌧GVI♫㸧〇ᕼ࢞ࢫ⏝ ࢔ ࣝ ࣑ ᐜ ჾ ୰ ࡟ ྛ ヨ ᩱࡢ ఩ ⨨ ࢆ グ 㘓 ࡋ ࡞㉁㔞ศᯒィVG3600 ࡟ࡼࡾ࢔ࣝࢦࣥྠ఩యẚࡀࡽࠊ✚ࡳ࠿ࡉࡡ࡚཰⣡ࡋࡓࠋࣇࣛࢵࢡࢫࣔ

ᐃࢆ⾜ࡗࡓࠋࢽ ࢱ ࡜ ࡋ ࡚ ࠊ ⡿ ᅜ ࢥ ࣟ ࣛ ࢻ ᕞ ⏘ ࡢ Fish

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㸱㸬◊✲ᡂᯝࣇ ࢕ ࣜ ࣆ ࣥ ᾏ ᆅ ᇦ ࠿ ࡽ ኱ 㝣 Ჴ 㝈 ⏺ ⏬ ᐃㄪᰝ࡟ࡼࡾ᥇ྲྀࡉࢀࡓヨᩱ࡟ࡘ࠸࡚ ᐃࢆ ᐇ ᪋ ࡋ ࡓ ࠋ ᖹ ᡂ 20 ᖺ ᗘ ࡣ JRR4 ࡢ ೵ Ṇࡢᙳ㡪࡛↷ᑕࡣ㸯ᅇ࡟࡜࡝ࡲࡾࠊ ᐃᩘࡶ㝈ࡽࢀࡓࠋ
ఀ㇋ᑠ➟ཎᘼす᪉ࠊᅄᅜᾏ┅୰࡟఩⨨ࡍࡿṊᒾ⁐ᒾࡢᖺ௦

⣖༡ᾏᗏᓴᆅᇦࡢ⋞Ṋᒾ࠿ࡽࡣ 11.8 ࠾ࡼࡧ2008 ᖺ 11 ᭶ᮎ࡟ㄽᩥᢞ✏ࢆ⾜ࡗࡓࠋᐃࢆ⾜ࡗࡓ⤖ᯝࠊ⫼ᘼᾏ┅ᣑ኱⤊஢ᚋ㸳Ѹ㸶㸮㸮୓ᖺᚋࡲ࡛ࡇࡢ≉Ṧ࡞ⅆᒣάືࡀ㉳ࡁ࡚࠸ࡓࡇ࡜ࢆ᫂ࡽ࠿࡟ࡋࡓࠋ
ࡉࡽ࡟௒ᖺᗘࡢ

ᐃ࡟ࡼࡾࠊᅄᅜᾏ┅ෆ࡛ୖグࡢⅆᒣάື࡜໬Ꮫⓗ≉ᚩࡀ඲ࡃ␗࡞ࡿࠊᓥ
ᘼⓗ࡞ⅆᒣάືࡀ࡯ࡰྠ᫬ᮇ࡟㉳ࡁ࡚࠸ࡓࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡗࡓࠋࡇࡢᡂᯝ࡟ࡘ࠸࡚

15.69Ma ࡢᖺ௦ࡀᚓࡽࢀࠊᾏᗏᓴࢆᵓᡂࡍࡿ᪥ ᮏ༡᪉ࣇ࢕ࣜࣆࣥᾏᆅᇦࡢⅆᒣάື2㸧᪥⋞Ṋᒾ㢮ࡀᅄᅜᾏ┅ᣑ኱೵Ṇ┤ᚋ࠿ࡽ 300 ୓ྐࠊᵓ㐀Ⓨ㐩ྐࡢゎ᫂ࢆ㏻ࡌࡓ኱㝣Ჴ㝈⏺⏬

ᖺ⛬ᗘࡢ㛫࡟άືࡋࡓࡇ࡜ࢆ♧ࡋ࡚࠸ࡿࠋ

ᐃ⏦ㄳ࡬ࡢ㈉⊩ 40 Ar/ 39 Arᖺ௦୍᪉⣖༡ᾏᒣิࡢᮾഃࠊ⣖༡ᾏᗏᓴࡢすഃᐃ࡟ࡼࡾࣇ࢕ࣜࣆࣥᾏ

࡟఩⨨ࡍࡿᓴ࠿ࡽ᥇ྲྀࡉࢀࡓ⋞Ṋᒾ࠿ࡽᆅᇦ඲య࠿ࡽ᥇ྲྀࡉࢀࡓᾏᗏᇶ┙ᒾࡢᙧᡂ

19.93 Ma ࡢᖺ௦ࡀᚓࡽࢀࡓࠋࡑࡢ⋞Ṋᒾࡣࠊᖺ௦ࢆ᫂ࡽ࠿࡟ࡋࡓࠋࡇࢀ࡟ࡼࡾࠊ᪥ᮏ༡᪉

ᅄᅜᾏ┅ᗏࢆᵓᡂࡍࡿ⋞Ṋᒾ࡜㢮ఝࡋࠊ୰ኸ

ᾏᇦࡢᆅ㉁ᵓ㐀ࡢᡂᅉ࡟ࡘ࠸࡚ከࡃࡢ㔜せᾏᕊ⋞Ṋᒾ࡟㏆࠸⤌ᡂࢆ♧ࡍࠋࡇࡢࡇ࡜࠿ࡽࠊ

࡞ไ⣙ࢆ୚࠼ࡓࠋࡇࢀࡽࡢࢹ࣮ࢱ࠾ࡼࡧゎ㔘ࡇࡢ⋞Ṋᒾࡣᅄᅜᾏ┅ᣑ኱ᮎᮇ࡟ࠊᾏ┅ᣑ኱

ࡣ 2008 ᖺ 11 ᭶࡟ᅜࡀᅜ㐃࡟ᥦฟࡋࡓ᪥ᮏࡢ࡟ క ࡗ ࡚ ά ື ࡋ ࡓ ࣐ ࢢ ࣐࡛ ࠶ ࡿ ࡜ ⪃ ࠼ ࡽ ࢀ኱㝣Ჴᘏఙࡢࡓࡵࡢ⏦ㄳ᭩࡟┒ࡾ㎸ࡲࢀࡓࠋࡿࠋᾏ┅ᣑ኱㍈௜㏆࠿ࡽ᥇ྲྀࡉࢀࡓࠊྠࡌࡃ

௒ᚋࡣࠊࣇ࢕ࣜࣆࣥᾏᆅᇦࡢᾏ┅ཬࡧྂᓥᘼ

୰ኸᾏᕊ⋞Ṋᒾ㢮ఝࡢ⋞Ṋᒾヨᩱ࡟ࡘ࠸࡚ࠊ

ࡢᙧᡂⓎ㐩ྐཬࡧ࣐ࣥࢺࣝࣉ࣮࣒ࣜࣗ࡜ᾏ

17.28Ma ࡢᖺ௦ࡀᚓࡽࢀࡓࠋࡇࡢ⤖ᯝࡶࠊࡇ┅ᙧᡂࡢ㛫ࡢᡂᅉⓗ㛵㐃➼࡟ࡘ࠸࡚ㄽᩥ໬ࡢ ⋞ Ṋ ᒾ ࡀ ᭱ ᮎ ᮇ ࡢ ᾏ ┅ᣑ ኱ ࡟ క ࡗ ࡚ ᙧ ᡂࡍࡿணᐃ࡛࠶ࡿࠋࡲࡓ௒ᚋྲྀᚓࡍࡿࢹ࣮ࢱࡣࠊ

ࡉࢀࡓࡇ࡜ࢆᙉࡃ♧၀ࡍࡿࠋᅜ㐃࡛ࡢ᪥ᮏࡢ⏦ㄳ᭩ࡢᑂᰝࢆࢧ࣏࣮ࢺࡍ
ࡿࢹ࣮ࢱ࡜࡞ࡿࠋす࣐ࣜ࢔ࢼᾏᕊ࠿ࡽ༡す᪉ྥ࡟ࡢࡧࡿᑠᾏ ᒣ ิ ୰ ࡢ ᾏ ᒣ ࠿ ࡽ ᚓ ࡽࢀ ࡓ ⋞ Ṋ ᒾ ࡟ ࡘ ࠸ཧ⪃ᩥ⊩

࡚ࠊ15.64Ma ࡢᖺ௦ࡀᚓࡽࢀࡓࠋࡇࢀࡣ,࣐ࣜ࢔ࢼᘼ⫼ᘼᆅᇦ࡟࠾࠸࡚ࡶࠊ⫼ᘼᾏ┅ᣑ኱

1㸧 Lanphere, M. A., Baadsgaard, H.,೵Ṇ࡜࡯ࡰྠ᫬࡟ࠊᓥᘼⅆᒣάືࡀ㉳ࡁ࡚࠸

2001. Precise K-Ar, Ar/ Ar, Rb-Sr andU/Pb mineral ages from the 27.5 Ma Fish
Canyon Tuff reference standard. Chem.
Geol. 175, 653-671.

40ࡓࡇ࡜ࢆ⿬௜ࡅࡿ⤖ᯝ࡛࠶ࡿࠋ
㸲㸬⤖ㄽ࣭⪃ᐹ391) ⫼ ᘼᾏ┅ᣑ኱⤊஢ᚋࡢ␗࡞ࡿࢱ࢖ࣉࡢ
ⅆᒣάືࡢඹᏑ ࣇ࢕ࣜࣆࣥᾏᆅᇦࡢ⫼ᘼᾏ┅㸦ᅄᅜᾏ┅ࠊࣃࣞࢫ࣋ࣛᾏ┅➼㸧ࡢ࠿ࡘ࡚ࡢᣑ኱㍈௜㏆࡟࠾࠸࡚ࠊ⫼ᘼᾏ┅ࡢ௚ࡢᆅᇦ࡛ࡣぢࡽࢀ࡞࠸

2) Ishizuka, O., Uto., K., Yuasa, M.,
2003. Volcanic history of the back-arc
region of the Izu-Bonin (Ogasawara)arc. Geol. Soc. Spec. Publ., 219,
187-205.

࢔ࣝ࢝ࣜ⋞ṊᒾࡢⅆᒣయࢆⓎぢࡋࡓࠋࡇࡢ⋞ཎᏊ⅔㸸JRR-3

⿦ ⨨㸸HRѸ㸰- 312 -

ศ 㔝㸸ᨺᑕ໬ศᯒ㸦ᆅ⌫໬Ꮫ㸧

3-1

JAEA-Review 2013-039

3-2࣓ࢫࣂ࢘࢔࣮ศගἲ࡟ࡼࡿ↓ᶵ໬ྜ≀ࡢ◊✲ VI
Mössbauer spectroscopic studies of inorganic compounds Part VIᮾ㑥኱Ꮫࠉ㧗ᶫࠉṇ㸪⥤㒊๛ஓ㸪᫬⏣⣪Ꮨ㸪἟㔝ဴᮁ㸪ᖹ஭ຬஓ㸪୕㡲ಇ⾜㸪௒஭࿴㈗㸦1㸧ࡣࡌࡵ࡟

࠸ࡓᙳ㡪ࢆ᳨ウࡋ࡚ࡁࡓ㸬௒ᮇࡣ㓄఩Ⅳ⣲ࢆྵࡴ࣓࣋ࢫࣂ࢘࢔࣮ศගἲࡣ 45 ඖ⣲㸪91 ᰾✀࡟ࡘ࠸࡚ほࣥࢮࣥ⎔ࢆࣇࢵ⣲໬ࡋࡓ࣍ࢫࣇ࢕ࣥ㘒య࡟ࡘ࠸࡚ࡢ

ࡉࢀࡿࡀ㸪㕲㸪ࢫࢬ࠾ࡼࡧࣘ࢘ࣟࣆ࣒࢘௨እࡢඖ
⣲࡟ࡘ࠸࡚ࡣ㸪ᕷ㈍ࡢ⥺※ࡀ࡞࠸ࡇ࡜ࡸప
ᾮయ❅⣲ᗘ௨ୗ㸧࡛ࡢ

◊✲ࢆ㐍ࡵࡓ㸬

㸦㏻ᖖ

ᐃࡀᚲせ࡞ࡓࡵ㸪໬Ꮫⓗ࡟ࡣ᭷⏝࡞᝟ሗࢆ୚࠼ࡿ࡜ᮇᚅࡉࢀ࡚ࡶ㸪◊✲࡟⏝࠸ࡽࢀ࡞࠸ඖ⣲ࡀᑡ࡞ࡃ࡞࠸㸬ࡇࡢ◊✲ࡣ㸪ࡑ࠺࠸ࡗࡓవࡾ࡞ࡌࡳࡢ࡞࠸ඖ⣲ࡢ࣓ࢫࣂ࢘࢔࣮ศගἲࢆ
⏝࠸࡚㸪⤖ྜࡸᵓ㐀࡟㛵ࡍࡿ᝟ሗࢆᚓࡿࡇ࡜ࢆ┠ⓗ࡜ࡋ࡚࠸ࡿ㸬ࡇࡢ 3 ᖺ㛫࡟ࢃࡓࡿ◊✲࡛ࡣ㸪(1) 197Au
࣓ࢫࣂ࢘࢔࣮ศගἲࢆ⏝࠸ࡓ㔠Ѝ࣍࢘⣲㏫౪୚⤖ྜࢆ ᣢ ࡘ ᭷ ᶵ 㔠 ໬ ྜ ≀ ࡸ ⎔≧ ᭷ ᶵ 㔠 㘒 య ࡢ ◊ ✲ 㸪(2)161Dy ࣓ࢫࣂ࢘࢔࣮ศගἲ࡟ࡼࡿࢪ࢝ࣝ࣎ࣥ㓟࡛ᯫᶫࡉࢀࡓ Dy 㘒యࡢ◊✲㸪(3) 155Gd ࣓ࢫࣂ࢘࢔࣮
ศගἲ࡟ࡼࡿ࢞ࢻࣜࢽ࣒࢘(III)–ࢺࣜࣇ࢙ࢽࣝ࣍ࢫ
ࣇ࢕ࣥ࢜࢟ࢩࢻ㘒యࡢ◊✲㸪(4) 170Yb ࣓ࢫࣂ࢘࢔࣮
ࢫ࣌ࢡࢺࣝᐃࡢࡓࡵࡢணഛᐇ㦂ࢆ࠾ࡇ࡞ࡗࡓ㸬㔠ᒓ㘒య࠶ࡿ࠸ࡣ᭷ᶵ㔠ᒓ໬ྜ≀࡟࠾࠸࡚ࡣ㸪㔠

(2)
197

197

ᒓ㸫㓄఩Ꮚ㛫ࡢ⤖ྜࡣ㓄఩Ꮚࡀ Lewis ሷᇶ㸪㔠ᒓཎ

Au ࣓ࢫࣂ࢘࢔࣮ศග

Au ࢫ࣌ࢡࢺࣝࡢ

ᐃࡣẚ㍑ⓗᐜ࡛᫆㸪ࡇࢀࡲ࡛ࡶከࡃࡢ◊✲ࡀ⾜ࢃࢀ࡚ࡁࡓ㸬ࢃࢀࢃࢀࡣ㸪⎔≧஧
197

Ꮚࡀ Lewis 㓟࡜ࡋ࡚┦஫స⏝ࡍࡿࡇ࡜࡟ࡼࡗ࡚࠸ࡿ㸬࡜ࡇࢁࡀ᭱㏆࣓ࣝ࢝ࣉࢺ࢖࣑ࢲࢰ࣮ࣝࡸ࣍ࢫࣇ࢕ࣥ

᰾㔠㘒యࡸ᭷ᶵ㔠໬ྜ≀ࡢ◊✲࡟㸪 Au ࣓ࢫࣂ࢘ࢆ⨨᥮ᇶ࡟ࡶࡘ࣎ࣛࣥ㓄఩Ꮚ(1, 2)ࡀタィࡉࢀ㸪ࡇ࢔࣮ࢫ࣌ࢡࢺࣝࢆ⏝࠸࡚ࡁࡓ㸬ࡢ㓄఩Ꮚ࡛ࡣ㓄఩Ꮚࡀ Lewis 㓟࡜ࡋ࡚స⏝ࡋ࡚㸪M

㔠ཎᏊࡣ㏻ᖖ+I ࡲࡓࡣ+III ࡢ㓟໬ᩘࢆ࡜ࡾ㸪ྠ᪘ЍB ⤖ྜࢆ⏕ᡂࡍࡿࡇ࡜ࡀ♧၀ࡉࢀ࡚ࡁࡓ㸬ࡇࡢࡼࡢ㖡࡜ࡣ㐪ࡗ࡚+II ࢆྲྀࡿࡇ࡜ࡣ㠀ᖖ࡟⌋ࡋ࠸㸬ᡃࠎ࠺࡞┦஫స⏝࡟ࡘ࠸࡚ࡣ㸪MЍBR3 ࡛࡞ࡃ M2+ЋBR32–

ࡣ㸪㛗࠸ࡇ࡜⎔≧஧᰾㔠(I)໬ྜ≀ࢆ✜ࡸ࠿࡟㓟໬ࡍ࡜ࡍࡿ⪃࠼ࡶᥦ᱌ࡉࢀ࡚࠾ࡾ㸪㟁Ꮚ≧ែࡢ᳨ウࡣ㔜ࡿ࡜㦵᱁ᵓ㐀ࢆಖᣢࡋࡓࡲࡲ⎔≧஧᰾㔠(II)㘒య࡜

せ࡞ㄢ㢟࡜࡞ࡗ࡚࠸ࡿ㸬ࡑࡇ࡛ Bourissou ࡽ࡟ࡼࡗ࡞ࡿࡇ࡜㸪࠾ࡼࡧࡇࢀࡣ୙ᆒ໬࡟ࡼࡾ Au(I, III)࡟࡞

࡚㛤Ⓨࡉࢀࡓ࣍ࢫࣇ࢓ࢽࣝ࣎ࣛࣥ PhB(C6H4PR2)ࡢ

ࡿࡇ࡜ࢆ♧ࡋ࡚ࡁࡓ㸬୍㐃ࡢ◊✲࡟࠾࠸࡚㸪

197

Au

㔠㘒య(2a, 2b)࡟ࡘ࠸࡚ 197Au ࣓ࢫࣂ࢘࢔࣮

ᐃࢆ⾜࣓ࢫࣂ࢘࢔࣮ศගἲࡣ㓟໬ᩘࡢỴᐃࡔࡅ࡛࡞ࡃ㸪㓄࡞࠸㸪Au–B ⤖ྜ࡟ࡘ࠸᳨࡚ウࡋࡓ㸬఩⎔ቃࡸ㟁Ꮚ≧ែࡢ㆟ㄽ࡟࠾࠸࡚᭷⏝࡛࠶ࡿࡇ࡜ࢆ

㹙ᐇ㦂㹛197Au ࣓ࢫࣂ࢘࢔࣮⥺※ࡣ㸪197Pt ࢆ JRR-3 PN♧ࡋ࡚ࡁࡓ㸬ࡇࢀࡲ࡛࡟㸪࣍ࢫࣇ࢕ࣥࡢ࣋ࣥࢮࣥ⎔↷ᑕᏍ࡛↷ᑕࡋ࡚సᡂࡋࡓ㸬ᮾ㑥኱ࡢప࡟࣓ࢳࣝᇶࢆᑟධࡋࡓຠᯝࡸ㸪㓄఩ཎᏊ࡟ࣄ⣲ࢆ⏝࢔ ࣮ ศ ග ჾ 㸦 Wissel ♫ ࡢ MDU-1200, MDV-1200,

࣓ࢫࣂ࢘◊✲᪋タ࣭⿦⨨㸸JRR-3M (PN-2, HR-1),◊✲ศ㔝㸸࣓ࢫࣂ࢘࢔࣮ศගἲ㸪㘒య໬Ꮫ㸪᭷ᶵ㔠ᒓ໬Ꮫ- 313 -

㻠

JAEA-Review 2013-039

DFG-1200 ࠿ࡽ࡞ࡿ㸧ࢆ⏝࠸࡚㸪100a 200 mgAu cm–2

ࣝ࠿ࡽ♧၀ࡉࢀࡿ㸬Au(I)㘒యࡶ Au(II)㘒యࡶ࣍ࢫࣇ

ࡢ྾཰యཌࡳࡢヨᩱ࡟ࡘ࠸࡚

ᐃࡋࡓ㸬㸯ᅇࡢ⥺※࢕ࣥ㘒యࡢሙྜࡼࡾࡶ IS, QS ࡜ࡶᑠࡉࡃ࡞ࡗ࡚࠸

ࡢసᡂ࡛㸪4a 5 ࢫ࣌ࢡࢺࣝࢆ

ᐃࡍࡿࡇ࡜ࡀ࡛ࡁ

ࡿࡀ㸪ࡇࢀࡣ࣋ࣥࢮࣥ⎔ࢆࣇࢵ⣲໬ࡋࡓᙳ㡪࡛࠶ࡾ㸪ࡓࠋ␗ᛶయࢩࣇࢺࡢ್ࡣ㸪⥺※ᇶ‽࡛⾲ࡋࡓࠋ໬ྜ

㟁Ꮚ౪୚⬟ࡢῶᑡࡀศ࠿ࡿ㸬ࡇࡢῶᑡࡣ㸪࣍ࢫࣇ࢕≀ࡣ㸪᪤ሗࡢ᪉ἲ࡟ࡼࡾྜᡂࡋࡓ㸬ࣥࢆ࢔ࣝࢩࣥ࡟௦࠼ࡓ࡜ࡁ࡟㏆࠸ࡀ㸪≉࡟ IS ࡢῶᑡࡢ࡯࠺ࡀ኱ࡁࡃ㸪Au 6s ㌶㐨࡬ࡢ౪୚⬟ࡀ௒ᅇࡢ

N
N

N
N

S
S

Ph

N

㘒య࡛ࡣῶᑡࡋࡓࡇ࡜ࡀ♧၀ࡉࢀࡿ㸬Au(II)㘒యࢆ

N

B

B
Au

PR2

⁐ ᾮ୰ ࡛ ຍ ⇕ࡋ ࡚ ᚓ ࡽࢀ ࡿ ⏕ ᡂ≀ ࡟ ࡣ 㸪Au(I) ࡜LnCl

R = iPr (2a)R = Ph (2b)Au(III)࡟ᖐᒓ࡛ࡁࡿ 2 ࢧ࢖ࢺࡀᏑᅾࡋ㸪୙ᆒ໬ࡀ㉳

1

2

M

S

R2P

ࡇࡗࡓࡇ࡜ࡀ☜ㄆ࡛ࡁࡿ㸬ࡑࡢ࣓ࢫࣂ࢘࢔࣮ࣃ࣓ࣛ

㹙⤖ᯝ࡜⪃ᐹ㹛ᚓࡽࢀࡓࢫ࣌ࢡࢺࣝࢆᅗ 1 ࡟♧ࡋࡓ㸬
I
2

Au 㸦F4-1㸧ࡣ୍⤌ࡢ኱ࡁ࡞ᅄᴟศ⿣㸦QS㸧ࢆᣢࡗII࣮ࢱࡣࡸࡣࡾ㸪ࣇࢵ⣲⨨᥮యࡣ IS ࡶ QS ࡶ࣍ࢫࣇ࢕ࣥ㘒యࡼࡾࡶᑠࡉࡃ࡞ࡗ࡚࠸ࡿ㸬I
2ࡓ஧㔜⥺㸪Au 2 ໬ྜ≀㸦F4-2㸧ࡣ Au ࡼࡾࡶᑠࡉ࡞
QS ࡢ஧㔜⥺࡛࠶ࡾ㸪஧ࡘࡢ Au ཎᏊࡀ➼౯࡛࠶ࡿࡇ࡜ࡀ☜ㄆ࡛ࡁࡓ㸬⇕ศゎ⏕ᡂ≀ F4-3 ࡣ஧⤌ࡢ஧㔜⥺࠿ࡽ࡞ࡾ㸪AuI–AuIII ࡢΰྜཎᏊ౯໬ྜ≀࡛࠶ࡿࡇ࡜ࡀ☜ㄆ࡛ࡁࡓ㸬

Fig. 2 197Au Mössbauer spectra of cyclo- metalated and related
complexes

Fig. 1

197

Au Mössbauer spectra of cyclometalated gold

compounds and their decomposition productsᅗ 2 ࡟⎔≧஧᰾㔠㘒యࡢ␗ᛶࢩࣇࢺ㸦IS㸧࡜ QS ࡢ㛵ಀࢆ♧ࡍ㸬㔠໬ྜ≀࡛ࡣ㸪㓟໬≧ែ࡟ࡼࡾ㸪IS
࡜ QS ࡀᅛ᭷ࡢ㡿ᇦ࡟ࣉࣟࢵࢺࡉࢀࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ㸬ฟⓎ≀㉁ࡢ஧᰾ Au(I)㘒యࡣ P,C-㓄఩ࡢࡓࡵ࡟኱ࡁ࡞ IS ࡜ QS ࢆ♧ࡍࡀ㸪ప࡛✜ࡸ࠿࡟㓟

໬ࡋ࡚⏕ᡂࡍࡿ஧᰾(II)㘒య࡛ࡣ㸪IS ࡶ QS ࡶῶᑡࡋ࡚࠸ࡿ㸬ࡇࢀࡣ Au(I)࠿ࡽ Au(II)࡟࡞ࡗࡓࡇ࡜࡟
క࠺㓄఩ᵓ㐀ࡢኚ໬࡟ࡼࡿࡶࡢ࡛࠶ࡿ㸬Au(II)໬ྜ
197≀࡛ࡣ㸪ࣁࣟࢤࣥࡔࡅ࡛࡞ࡃᏳᜥ㤶㓟࢖࢜ࣥࡸ◪㓟

Fig. 3࢖࢜ࣥࡶ㓄఩ࡋ࡚࠸ࡿࡇ࡜ࡀ࣓ࢫࣂ࢘࢔࣮ࢫ࣌ࢡࢺ

complexes.

- 314 -

Au Mössbauer spectra of gold-phosphanylborane

3-2
㻡JAEA-Review 2013-039

ࠉ࣍ࢫࣇ࢓ࢽࣝ࣎ࣛࣥ㘒య 2a, 2b ࡢ 12 K ࡛ࡢࢫ࣌ࢆసࡾฟࡍࡓࡵ࡟ᗈࡃ◊✲ࡉࢀ࡚ࡁࡓ㸬ᡃࠎࡣⰍࠎ

ࢡࢺࣝࢆᅗ 3 ࡟♧ࡋࡓ㸬࣓ࢫࣂ࢘࢔࣮ࣃ࣓࣮ࣛࢱࡣ

࡞㙐㛗ࡢ⬡⫫᪘ࢪ࢝ࣝ࣎ࣥ㓟–O2C(CH2)nCO2–㸦n = 0

IS = 3.40, QS = 7.73 mm s–1 (2a), IS = 3.31, QS = 7.53

a 5㸧ࡢࣛࣥࢱࣀ࢖ࢻ㘒యࡢḟඖᛶ࡟⯆࿡ࢆࡶࡕ㸪

mm s

–1

(2b)࡛࠶ࡗࡓ㸬ࡇࢀࡽࡢࣃ࣓࣮ࣛࢱࡢ IS ࡜

Dy(III)㘒యࡢ࣓ࢫࣂ࢘࢔࣮ࢫ࣌ࢡࢺࣝࢆ

ᐃࡋࡓ㸬㹙ᐇ㦂㹛ࢩࣗ࢘㓟㸦n = 0; H2ox㸧㸪࣐ࣟࣥ㓟㸦n = 1;

QS ࡢ㛵ಀࢆ♧ࡍ࡜ᅗ 4 ࡢࡼ࠺࡟࡞ࡿ㸬㸪ࢥࣁࢡ㓟㸦n = 2; H2suc㸧㸪ࢢࣝࢱࣝ㓟㸦n = 3;H2mal㸧
H2glu㸧
㸪࢔ࢪࣆࣥ㓟㸦n = 4; H2adi㸧㸪ࣆ࣓ࣜࣥ㓟㸦n =5; H2pim㸧㸪ࣜࣥࢦ㓟㸦H2mali㸧ࡢ㘒య Ln2L3·xH2O
ࡣ㸪DyCl3 Ỉ⁐ᾮ࡟ࢪ࢝ࣝ࣎ࣥ㓟ࢆຍ࠼࡚ pH ࢆ 4.5
a 5.5 ࡟ㄪ〇ࡋ࡚ྜᡂࡋࡓ㸬㔜㔞ศᯒ࡟ࡼࡾ㘒యࡢ⤌ ᡂ ࢆ ḟ ࡢ ࡼ ࠺ ࡟ Ỵ ᐃ ࡋ ࡓ 㸬 Dy2(ox)3·10H2O 㸪
Dy2(mal)3·6H2O 㸪 Dy2(suc)3·2H2O 㸪 Dy2(glu)3·2H2O 㸪
Dy2(adi)3·2H2O㸪Dy2(pim)3·5H2O㸪Dy2(mali)3·2H2O㸬
161
160

Dy ࣓ࢫࣂ࢘࢔࣮⥺※ 161Tb/GdF3㸦273 MBq㸧ࡣ

Gd2O3 ࡜ NH4F ࡢᅛ┦཯ᛂ࡛ྜᡂࡋࡓ 160GdF3 ࢆ㸪

JRR-3 HR-2 ↷ᑕᏍ࡛ 20 h ୰ᛶᏊ↷ᑕࢆࡋ࡚సᡂࡋ
Fig. 4

IS-QS plot of gold-phophanylborane complex. IS

values are relative toࡓ㸬ࢫ࣌ࢡࢺࣝࡣ㸪25.7 keV ࡢ࣓ࢫࣂ࢘࢔࣮Ț⥺ࢆẚ౛ィᩘ⟶㸦Xe-CO2㸧࡛ィ

metallic Au.

ᅗ 4 ࡟ࡣ㸪✀ࠎࡢ Au(I)࠾ࡼࡧ Au(III)㘒య࡟ࡘ࠸–2

cm ࡜࡞ࡿヨᩱࢆ⏝࠸࡚ࡋ࡚ᐃࡋࡓ㸬50 mgDy

ᐃࡋࡓ㸬Wissel ♫ࡢ࣓ࢫ࡚ࡢ IS࡜ QSࡢ㛵ಀࡶࣉࣟࢵࢺࡉࢀ࡚࠸ࡿ㸬2a㸪2bࣂ࢘࢔࣮㥑ື⿦⨨ࢆ⏝࠸ࢫ࣌ࢡࢺࣝࢆ

࡜ࡶ࡟㸪Au(I)ࡢ㡿ᇦ࡟఩⨨ࡋ࡚࠸ࡿ㸬ࡇࡢࡇ࡜࠿

㏿ᗘ㸦s100 mm s–1㸧ࡣ࣮ࣞࢨᖸ΅ィࢆ⏝࠸࡚

III

2–

I

ᐃࡋ㸪㥑ື
ᐃ

ࡽ㸪Au–B ⤖ྜࡣ Au ЋBR3 ࡛࡞ࡃ Au ЍBR3 ࡛࠶ࡋࡓ㸬ࢫ࣌ࢡࢺࣝࡢゎᯒࡣ㸪Ig = 5/2 ࡜ Ie = 5/2 㛫ࡢࡾ㸪࣎ࣛࣥ㓄఩Ꮚࡀ㟁Ꮚཷᐜయ࡜ࡋ࡚ാ࠸࡚࠸ࡿࡇ

ᅄᴟ㑄⛣࡟ࡘ࠸࡚㸪㠀ᑐ⛠ᐃᩘ = 0 ࡜ࡋ࡚⾜ࡗࡓ㸬࡜ࡀ᫂☜࡟࡞ࡗࡓ㸬࡜ࡇࢁ࡛ࡇࢀࡽࡢ㘒యࡣ
AuIP2BCl ࡢᖹ㠃ᅄ㓄఩ᆺ㓄⨨ࢆྲྀࡗ࡚࠸ࡿ㸬Au(I)ࡣ㏻ᖖ┤⥺ 2 㓄఩ࢆ࡜ࡿࡢ࡛ࡇࡢᵓ㐀ࡣ⌋ࡋࡃ㸪ẚ
㍑ᑐ㇟࡜࡞ࡿ AuI ໬ྜ≀ࡢࢹ࣮ࢱࡀᏑᅾࡋ࡞࠸㸬ࡑ
ࡇ࡛Ⅼ㟁Ⲵᶍᆺ࡛ࡣ㸪ᖹ㠃 4 㓄఩໬ྜ≀ࡢ㒊ศᅄᴟศ⿣ࡣ┤⥺ᵓ㐀ࡢ 1/2 ࡟࡞ࡿࡇ࡜ࢆ຺᱌ࡋ࡚ࣃ࣓࣮ࣛࢱࢆぢ࡚ࡳࡿ࡜㸪࡯ࡰྜ⌮ⓗ࡞್࡟ぢ࠼ࡿ㸬(3) 161Dy ࣓ࢫࣂ࢘࢔࣮ศග
161

Dy ࡢ࣓ࢫࣂ࢘࢔࣮⥺ࡢ࢚ࢿࣝࢠ࣮ࡣ 25.7 keV ࡜ప࠸ࡓࡵ࡟㸪ᐊ࡛ࡶ࣓ࢫࣂ࢘࢔࣮ຠᯝࡀほ࡛ࡁࡿ㸬ࡇࡢࡇ࡜࡜㸪⊃࠸⥺ᖜ࡜኱ࡁ࡞᰾☢Ẽ࣮࣓ࣔࣥࢺࢆᣢࡘࡓࡵ࡟㸪☢ᛶయ࡞࡝ࡢ≀ᛶ◊✲࡟᭷⏝࡛࠶ࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ㸬ࡋ࠿ࡋ↓ᶵ໬Ꮫⓗ࡞どⅬ࡛ࡢ◊✲ࡣ௨እ࡜ᑡ࡞࠸㸬ࠉࣛࣥࢱࣀ࢖ࢻࡢ㓄఩㧗ศᏊࡣ㏆ᖺ㸪☢ᛶయ㸪Ⓨගᮦᩱ㸪ศᏊໟ᥋యࡸゐ፹࡞࡝ࡢከᏍᛶ≀㉁࡜ࡋ࡚ὀ
┠ࢆ㞟ࡵ࡚࠸ࡿ㸬ᯫᶫ㓄఩Ꮚ࡜ࡋ࡚ࡢࢪ࢝ࣝ࣎ࣥ㓟㸪≉࡟⬡⫫᪘ࢪ࢝ࣝ࣎ࣥ㓟ࡣ㸪ᰂ㌾࡟ከᵝ࡞⤖ᬗᵓ㐀

Fig. 5 161Dy Mössbauer spectra of DyIII–dicarboxylates at 77 K

3-2
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JAEA-Review 2013-039

၀ࡋ࡚࠸ࡿ㸬ࡇࡢ◊✲࡛⏝࠸ࡓ㘒యࡢ⤖ᬗᵓ㐀ࡣ᫂ࡽ࠿࡟࡞ࡗ࡚࠸࡞࠸ࡀ㸪୍⯡࡟ࢩࣗ࢘㓟࢖࢜ࣥࡣ㔠ᒓ୰ᚰ㛫ࢆᯫᶫࡋࡓ 3 ḟඖⓗࢿࢵࢺ࣮࣡ࢡࢆసࡾࡸ
ࡍ࠸ࡇ࡜ࡸ㸪㙐㛗ࡀ㛗࠸ࢪ࢝ࣝ࣎ࣥ㓟㘒యࡣ㸪㏻ᖖ
2 ḟඖⓗ࡞ pillared layer ᵓ㐀ࢆྲྀࡿࡇ࡜ࢆ⪃࠼ࡿ࡜㸪ྜ⌮ⓗ࡜࠸࠼ࡿ㸬ࢢࣝࢱࣝ㓟㘒య࡟ࡘ࠸࡚ࡣ㸪 ᗘኚ໬ࢆᐃࡋ㸦ᅗ7㸧㸪㠃✚ᙉᗘ࠿ࡽ᱁ᏊຊᏛⓗࣃ࣓࣮ࣛࢱ M2 ࢆồࡵࡓ㸬M2 = 4.64106 g mol–1 K–1 ࡛࠶ࡾ㸪ࢹࣂ࢖
ᗘࡣ 110 K ࡜ぢ✚ࡶࡽࢀࡓ㸬ࡇࡢ್ࡣࢩ࢔ࣀᯫᶫ
3ḟ ඖ 㓄 ఩ 㧗 ศ Ꮚ
2

DyFe(CN)4·4H2O

ࡸ6

Fig. 6 Relation between absorption area and the number of

KDyFe(CN)6·4H2O ࡢ M ࡢ್ 7.410 ࠾ࡼࡧ 6.3106

methylene group n in dicarboxylate anion

g mol–1 K–1 ࡼࡾࡣᑠࡉࡃ㸪᭱㏆ᡃࠎࡀ

ᐃࡋࡓ 2 ḟඖ㓄఩ Eu(III)㘒య 4.6710 (M = Ni), 4.78106 (M =6Co), 6.30106 g mol–1 K–1 (M = Mn)࡜ྠ⛬ᗘ࡛࠶ࡾ㸪ᡃࠎࡀ᥎ᐃࡋ࡚࠸ࡿ pillared layer ᵓ㐀࡜▩┪ࡋ࡞࠸㸬

Fig. 8161

Dy Mössbauer spectra of Dy2(glu)3·2H2O simulated

by Nowick-Wickman’s model.

ࠉࢢࣝࢱࣝ㓟㘒యࡢࢫ࣌ࢡࢺࣝࡢ⥺ᙧࡣ⦆࿴ࢫ࣌ࢡ

Fig. 7 Temperature dependence of Dy2(glu)3·2H2O–2㹙⤖ᯝ࡜⪃ᐹ㹛50 mgDy cm ࡢヨᩱ࡟ࡘ࠸࡚

ᐃࡋࢺࣝ࡟ぢ࠼ࡿࡢ࡛㸪Nowick-Wickman ࡢࢫࣆࣥ⦆࿴

ࡓ 77 K ࡛ࡢࢫ࣌ࢡࢺࣝࢆᅗ 5 ࡟♧ࡍ㸬ྠࡌ྾཰య

ᶍᆺࢆ⏝࠸࡚ゎᯒࡋࡓ㸦ᅗ 8㸧
㸬77 K ࡟࠾ࡅࡿ⦆࿴

ཌࡳ࡛ᐃࡋ࡚࠸ࡿࡀ㸪ࢪ࢝ࣝ࣎ࣥ㓟ࡢ㙐㛗 n ࡀ㛗᫬㛫ࡣ 30 ps ࡛࠶ࡾ㸪160 K ࡛ࡣ 0.2 ps ࡲ࡛▷ࡃ࡞ࡃ࡞ࡿ࡟ࡘࢀ࡚྾཰ᙉᗘࡀᙅࡃ࡞ࡿࡇ࡜ࡀࢃ࠿ࡿ㸬ࡗࡓ㸬⦆࿴᫬㛫ࡣࢫࣆࣥ㛫ࡢ㊥㞳࡟㛵ಀࡍࡿࡇ࡜ࡀ

㠃✚ᙉᗘ࡜㙐㛗 n ࡢ㛵ಀࢆᅗ 6 ࡟♧ࡍ㸬n = 0㸦ࢩ▱ࡽࢀ࡚࠸ࡿ㸬ࡇࡢ㘒యࡢ Dy3+–Dy3+㊥㞳ࡣ୙࡛᫂ࣗ࢘㓟㸧࠿ࡽࢥࣁࢡ㓟㸦n = 2㸧ࡢ㛫࡛ᛴ⃭࡟ῶᑡ࠶ࡿࡀ㸪ከࡃࡢ Dy(III)–ࢪ࢝ࣝ࣎ࣥ㓟㘒య࡛ࡣ 400ࡋ࡚࠸ࡿࡀ㸪n = 2 ௨ୖ࡛ࡣࡑࢀ࡯࡝኱ࡁࡃኚ໬ࡋ

㸫450 pm ࡛࠶ࡾ㸪ࡇࡢ㘒యࡶྠᐃࡢ㊥㞳ࢆᣢࡘ࡜࡞࠸㸬ࡇࢀࡣ▷࠸㙐㛗ࡢࢪ࢝ࣝ࣎ࣥ㓟㘒యࡣࣜࢪࢵ

᥎ᐃࡉࢀࡿ㸬௨๓࡟◊✲ࡋࡓ Er(III)–-ࢪࢣࢺࣥ㘒ࢻ࡞⤖ᬗᵓ㐀ࢆྲྀࡗ࡚࠸ࡿࡀ㸪㙐㛗ࡀ㛗ࡃ࡞ࡿ࡜ࣜ

య㸦12 K㸧࡛ࡣ㸪Er3+–Er3+ = 558 pm ࡢ࡜ࡁ = 400 ps,ࢪࢵࢻࡉࡀῶᑡࡋࡓ⤖ᬗᵓ㐀࡜࡞ࡗ࡚࠸ࡿࡇ࡜ࢆ♧Er3+–Er3+ = 587 pm ࡛ 500 ps, Er3+–Er3+ = 382 pm ࡛ 100

3-2- 316 -

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JAEA-Review 2013-039

ps ࡛࠶ࡗࡓ㸬┤᥋ࡢẚ㍑ࡣ࡛ࡁ࡞࠸ࡀ㸪Er(III)--ࢪࡘ࠸࡚㸪࣮ࣟࣞࣥࢶᆺ㛵ᩘࢆ⏝࠸࡚⾜࡞ࡗࡓ㸬Gdࢣࢺࣥ㘒యࡢሙྜ࡜ࡼ࠸ᑐᛂࢆࡋ࡚࠸ࡿ㸬ࡣ⥺※ᇶ‽࡛⾲ࢃࡋࡓ㸬㹙⤖ᯝ࡜⪃ᐹ㹛Eu 㘒యࡢ㐣ሷ⣲㓟ሷ㸦3-Eu-A ࡜ᶆ

(3)

155

グ㸧࠾ࡼࡧ◪㓟ሷ㸦3-Eu-B ࡜ᶆグ㸧ࡢ 77 K ࡛ࡢ 151Eu

Gd ࣓ࢫࣂ࢘࢔࣮ศග

Gd ࣓ࢫࣂ࢘࢔࣮ࢫ࣌ࢡࢺࣝࡢ≉Ⰽࡣ㸪␗ᛶయࢩᅄᴟ⤖ྜᐃᩘ e2qQEu
࣓ࢫࣂ࢘࢔࣮ࣃ࣓࣮ࣛࢱࡣ㸪Eu㸪ࣇࢺ࡜ᅄᴟ⤖ྜᐃᩘ࠿ࡽ㸪㟁Ⲵศᕸࡸ⤖ྜ࡟ࡘ࠸࡚

ࡢ㡰࡟㸪0.20, 5.36 mm s–1 (3-Eu-A)㸪0.30, 3.68 mm s–1

ࡢ㆟ㄽࡀ࡛ࡁࡿࡇ࡜࡟࠶ࡿ㸬ࡇࢀࡲ࡛࡟-ࢪࢣࢺࣥ㸪(3-Eu-B)࡛࠶ࡗࡓ㸬Eu ࡢ್ࡣ㸪3-Eu-A ࡣ 8 㓄఩࡜

EDTA㸪࣏࢚ࣜࢳࣞࣥࢢࣜࢥ࣮ࣝ࡞࡝ࡢ Gd(III)㘒యࡋ࡚ࡣᑠࡉࡵ࡛࠶ࡿࡀ㸪ጇᙜ࡞್࡛࠶ࡗࡓ㸬3-Gd-

࠾ࡼࡧ CN ᯫᶫ Gd(III)㓄఩㧗ศᏊ࡞࡝ࡢ࣓ࢫࣂ࢘࢔

A ࡜ 3-Gd-B ࡢ 155Gd ࣓ࢫࣂ࢘࢔࣮ࣃ࣓࣮ࣛࢱࡣGd,࣮ࢫ࣌ࢡࢺࣝࡢ⣔⤫ⓗ࡞◊✲࠿ࡽ㸪❅⣲ཎᏊࡀ㓄఩

e2qQGd ࡢ㡰࡟㸪0.67, 6.63 (3-Gd-A), 0.61, 1.99 (3-Gd-ࡍࡿ࡜␗ᛶయࢩࣇࢺࡀᑠࡉࡃ࡞ࡿഴྥࢆぢ࠸ࡔࡋ࡚B)࡛࠶ࡗࡓ㸬Gd 㘒య࡛ 9 㓄఩ࡢ 3B ࡢ᪉ࡀ e2qQ ࡀ࠸ࡿ㸬ᑠࡉࡃ࡞ࡗ࡚࠸ࡿࡢࡣ㸪࠾ࡑࡽࡃ㓄఩ᩘࡢቑຍ࡟క

ࠉࢺࣜ࢜ࢡࢳࣝ࣍ࢫࣇ࢕ࣥ࢜࢟ࢩࢻ㸦TOPO㸧࡟௦࠸㟁Ⲵศᕸࡢᑐ⛠ᛶࡀቑຍࡋࡓࡓࡵ࡜ᛮࢃࢀࡿ㸬ࡇ⾲ࡉࢀࡿ࣍ࢫࣇ࢕ࣥ࢜࢟ࢩࢻ㢮ࡣ⁐፹ᢳฟ࡟࠾࠸࡚㸪ࢀ࡟ᑐࡋ 3A ࡢ EFG ࡀ኱ࡁ࠸ࡢࡣ㸪㓄఩Ꮚࡢ TPPO㔜せ࡛࠶ࡾ㸪⁐፹ᢳฟࡸ⁐ᾮ໬Ꮫ࠿ࡽከᩘࡢ◊✲ࡀ

࡜ ClO4– ࡢࡶࡘ㟁Ⲵࡀ㐪࠺ࡇ࡜࡜㸪஧ࡘࡢ ClO4– ࡀ⾜࡞ࢃࢀ࡚ࡁࡓ㸬ࢃࢀࢃࢀࡣᅛయ໬Ꮫⓗ࡞どⅬ࠿ࡽ

Ln3+ࢆᣳࢇ࡛┤⥺ⓗ࡟఩⨨ࡋ࡚࠸ࡿࡇ࡜࡞࡝࡟ࡼࡿ

࣍ࢫࣇ࢕ࣥ࢜࢟ࢩࢻ㢮ࡢ◊✲ࢆጞࡵࡓ㸬TOPO 㘒య

࡜ᛮࢃࢀࡿ㸬Eu(III)㘒య࡛ࡣ 7Fn Ћ5D0 ࡢⓎගࡀほࡣ⤖ᬗᛶࡀࡼࡃ࡞࠿ࡗࡓࡢ࡛㸪ࢺࣜࣇ࢙ࢽࣝ࣍ࢫࣇ

ࡉࢀࡿࡀ㸪Ⓨගࢫ࣌ࢡࢺࣝ࠿ࡽ 3-Eu-B ࡣ 3-Eu-A

࢕ ࣥ ࢜ ࢟ ࢩ ࢻ 㸦 TPPO 㸧 ࢆ ⏝ ࠸ ࡚ 㘒 య ࢆ ྜ ᡂ ࡋ ,ࡼࡾࡶᒁᡤⓗ࡞ᑐ⛠ᛶࡀ㧗࠸ࡇ࡜ࡀ♧၀ࡉࢀ࡚࠾ࡾ㸪Ln(tppo)4(ClO4)3ROH㸦3A; Ln = La, Nd, Eu, Gd, Dy,࣓ࢫࣂ࢘࢔࣮ࢫ࣌ࢡࢺࣝࡢ⤖ᯝ࡜୍⮴ࡋ࡚࠸ࡿ㸬155

Yb㸧࠾ࡼࡧ Ln(tppo)2(NO3)3EtOH㸦3B; Ln = Eu, Gd㸧
ࢆᚓࡓ㸬X ⥺ᵓ㐀ゎᯒ࠿ࡽ๓⪅ࡣ⯆࿡῝࠸ࡇ࡜࡟ 2
ศᏊࡢ ClO4–ࡀ࣮࢟ࣞࢺࡋࡓ 8 㓄఩༑஧㠃యᆺ㘒య
[Ln(tppo)4(2-O2ClO2)2]ClO4_ROH㸦Nda Yb 㘒యࡣྠᙧ㸧࡛࠶ࡿࡇ࡜ࡀࢃ࠿ࡗࡓ㸬Ln–O2ClO2 ㊥㞳㸦250
a 264 pm㸧ࡣ Ln–tppo ࡼࡾࡶ 27a 30 pm ࡯࡝㛗ࡃ㸪
ClO4– ࡢ 㓄 ఩ ࡣ ᙅ ࠸ ࡇ ࡜ ࡀ ♧ ࡉ ࢀ ࡓ 㸬
Ln(tppo)2(NO3)3EtOH ࡣ୕ࡘࡢ NO3– ࡀ࣮࢟ࣞࢺࡋࡓ
9 㓄఩㘒య࡛࠶ࡗࡓ㸬ࡇࡢㄢ㢟࡛ࡣ㸪ྠᙧࡢ⤖ᬗࢆసࡿ Eu ࡜ Gd 㘒యࡢ TPPO 㘒య࡟ࡘ࠸࡚㸪151Eu ࠾

Fig. 9 155Gd (left) and 151Eu (right) Mössbauer spectra of Ln-

ࡼࡧ 155Gd ࣓ࢫࣂ࢘࢔࣮TPPO complexesᐃࢆ⾜࡞࠸㸪ẚ㍑᳨ウࢆ

e2qQ ࡢ್࠿ࡽ Eu㸪Gd ୧㘒యࡢ EFG Vzz ࢆồࡵࡿヨࡳࡓ㸬㹙ᐇ㦂㹛LnX3·nH2O (Ln = La, Nd, Eu, Gd, Dy, Yb; X =࡜㸪3-Eu-A ࡜ 3-Gd-A ࡣ 3.371021, 3.661021 V m–2

ClO4–, NO3–) ࡢ ROH㸦R = Me, Et㸧⁐ᾮ࡟ 4 ಸࣔࣝ࡜࡯ࡰ୍⮴ࡍࡿࡢ࡟㸪3-Eu-B ࡜ 3-Gd-B ࡣ 2.321021,

ࡢ TPPO ࡢ ROH ⁐ᾮࢆຍ࠼㸪ROH ࢆ⵨Ⓨࡉࡏࡿ࡜

1.101021 V m–2 ࡜ᕪࡀぢࡽࢀࡓ㸬EFG ࡀᑠࡉ࡞ 3B

㘒యࡀᚓࡽࢀࡓ㸬࡛ᕪࡀぢࡽࢀࡿࡢࡣ㸪Gd(III)ࡣ 4f7 ࡛⤖ᬗሙࡢᙳ㡪ࠉ⥺※ࡣ᪤࡟ሗ࿌ࡋࡓ⥺※㸪ࡍ࡞ࢃࡕ JRR-3 HR-1ࡀ↓ど࡛ࡁࡿࡢ࡟ᑐࡋ࡚㸪4f6 ࡢ Eu(III)࡛ࡣ୍ࡘᏑ

࡛ 67 h ↷ᑕࡋ࡚సᡂࡋࡓ 155Eu/SmPd3㸦༙ῶᮇ 4.96

ᅾࡍࡿ 4f ࣮࣍ࣝࡢࡓࡵ࡟⤖ᬗሙࡢຠᯝࡀᏑᅾࡋ㸪y㸧ࢆ⏝࠸࡚

ࡇࢀࡀ᱁Ꮚࡢ EFG ࡟ᑐࡍࡿᐤ୚ࡀᑠࡉࡃ࡞ࡗࡓࡓ

ᐃࡋࡓ㸬 ᐃࡣ㸪⥺※࡜ヨᩱ㸦80 mgGd–2

cm 㸧ࢆ 12 K ࡟෭༷ࡋ࡞ࡀࡽ㸪Wissel ♫ࡢ 1200 㥑ືࢩࢫࢸ࣒ࢆ౑ࡗ࡚࣮ࢨᖸ΅ィ࡛

ࡵ࡟㢧ᅾ໬ࡋࡓࡓࡵ࡜⌧ᅾࡢ࡜ࡇࢁ⪃࠼࡚࠸ࡿ㸬ᐃࡋࡓ㸬⥺※ࡢ㥑ື㏿ᗘࡣࣞ

3-2ᐃࡋࡓ㸬ゎᯒࡣ㸪5/2–3/2 ࡢ㑄⛣࡟

- 317 -

㻤

JAEA-Review 2013-039(4) 170Yb ࣓ࢫࣂ࢘࢔࣮ศග

࡞ࡗ࡚࠸ࡿࡢࡣ㸪ࣛࣥࢱࢽࢻ཰⦰࡟ࡼࡗ࡚⤖ᬗ᱁Ꮚ࢖ࢵࢸࣝࣅ࣒࢘ࡣ㔜ᕼᅵ࡟ᒓࡋ㸪Eu ࡯࡝࡛ࡣ࡞࠸

ࡀᑠࡉࡃ࡞ࡗࡓࡓࡵ࡜⪃࠼ࡽࢀࡿࡀ㸪Yb2O3 ࡜ Gd2O3

ࡀ+2 ౯ࢆྲྀࡾࡸࡍ࠸ඖ⣲࡛࠶ࡾ㸪࣓ࢫࣂ࢘࢔࣮ࢫ

࡛ࡣ C3 ࡜ C2 ࢧ࢖ࢺࡢ㟁ሙ໙㓄ࡢ኱ࡁࡉࡀ㏫࡟࡞ࡗ

࣌ࢡࢺࣝ࠿ࡽᚓࡽࢀࡿ᝟ሗࡣ㸪໬Ꮫ⤖ྜࡸᵓ㐀࡟ࡘ࡚࠸ࡿ㸬ࡑࡢཎᅉࡣ୙࡛᫂࠶ࡿ㸬࠸࡚᭷⏝࡛࠶ࡿ࡜ᮇᚅ࡛ࡁࡿ㸬Yb ࡢ࣓ࢫࣂ࢘࢔࣮
ຠᯝࡣ 5 ᰾✀ 6 㑄⛣࡟ࡘ࠸࡚▱ࡽࢀ࡚࠸ࡿࡀ㸪࣓ࢫࣂ࢘࢔࣮᰾≉ᛶ࡜⥺※ࡢㄪ〇ࡢࡋࡸࡍࡉ࠿ࡽ㸪170Yb
ࡀ㐺ࡋ࡚࠸ࡿ㸬
ࠉ170Yb ࡢ࣓ࢫࣂ࢘࢔࣮㑄⛣ࡣ E = 84.26 keV ࡢ Ig = 0
࡜ Ie = 2 ࡢ㛫ࡢ E2 㑄⛣࡛࠶ࡾ㸪ບ㉳≧ែࡢᑑ࿨ࡣ 1.5
ns㸦Wo = 2.08 mm s–1㸧࡛࠶ࡿ㸬ࡇࢀࡽࡢ≉ᛶࡣ 166Er࡟ఝ࡚࠾ࡾ㸪᪤࡟⾜ࡗࡓ 166Er ࣓ࢫࣂ࢘࢔࣮ศගࡢ
⤒㦂ࢆ⏕࠿ࡍࡇ࡜ࡀ࡛ࡁࡿ㸬㹙ᐇ㦂㹛࣓ࢫࣂ࢘࢔࣮⥺※࡟ࡣ 170Tm/Al2Tm ࢆ౑⏝ࡋࡓ㸬Al2Tm ࡣ໬Ꮫ㔞ㄽẚࡢ Al ࡜ Tm ࢆ࢔࣮ࢡ⁐⼥ࡋ࡚࠿ࡽࢹ࢕ࢫࢡ≧࡟ษࡾฟࡋࡓ㸬Al2Tm 92 mg
ࢆ JRR-3 HR-2 ↷ᑕᏍ㸦th = 5.51013 cm–2 s–1㸧࡛ 55ศ㛫↷ᑕࡋ࡚సᡂࡋࡓ㸬࣓ࢫࣂ࢘࢔࣮

ᐃࡣ㸪170Tm

Fig. 10 170Yb and 155Gd Mössbauer spectra of Yb2O3 and Gd2O3

㸦t1/2 = 128.6 d㸧ࡢ 84.26 keV ࡢȚ⥺ࢆ LEPS ࡛ィᩘࡋ࡚࠾ࡇ࡞ࡗࡓ㸬ᐃࡣ Wissel ♫〇 1200 ࣓ࢫࣂ࢘(5) ௒ᚋࡢィ⏬

࢔࣮ࢩࢫࢸ࣒ࢆ⏝࠸㸪⥺※࡜྾཰యࢆ 20 K ࡟෭༷

ཎᏊ⅔ࢆ⏝࠸࡚࣓ࢫࣂ࢘࢔࣮⥺※ࢆసᡂࡋ࡚໬Ꮫⓗࡋ࡚࠾ࡇ࡞ࡗࡓ㸬⥺※ࡢ㥑ື㏿ᗘࡣ࣮ࣞࢨ࣮ᖸ΅ィ࡟᭷⏝࡞▱ぢࢆ୚࠼ࡿ࣓ࢫࣂ࢘࢔࣮ศගᏛⓗ◊✲ࢆ࡛㐍ࡵࡿ࡜࠸࠺ᙜึࡢ┠ⓗࡣ฿㐩ࡉࢀ࡚࠸ࡿ࡜⪃࠼࡚ᐃࡋࡓ㸬Yb2O3 ࡛ࡣ 1 ࢫ࣌ࢡࢺࣝࡢ

ᐃ࡟ 7a 8170࠸ࡿ㸬௒ᚋࡶᕼᅵ㢮◊✲ࡢࡓࡵ࡟ 155Gd ࡸ 161Dy㸪
Yb

᪥ࢆせࡋࡓ㸬

ᐃࢆ⥆ࡅ࡚⾜ࡃணᐃ࡛࠶ࡿ㸬170Yb ࡟ࡘ࠸࡚ࡣࡲ

㹙⤖ᯝ࡜⪃ᐹ㹛ጞࡵ࡟ Yb2O3 ࢆ⏝࠸࡚྾཰యཌࡳ࡟
ࡼࡿࢫ࣌ࢡࢺࣝࡢ㐪࠸ࢆ☜ㄆࡍࡿࡓࡵ࡟ 56 a–2ࡔᐃࡀ࡛ࡁࡿࡇ࡜ࡀ☜ㄆ࡛ࡁࡓẁ㝵࡛࠶ࡿࡀ㸪໬ᐃࡋ㸪௨㝆ࡣ 112 mgYbᏛⓗ࡞ᛂ⏝ࢆ㐍ࡵ࡚⾜ࡁࡓ࠸㸬197Au ࡟ࡘ࠸࡚ࡣ㸪ᐃࡍࡿࡇ࡜࡟ࡋࡓ㸬ࡇࡢ྾཰యཌ

᭷ᶵ㔠ᒓ໬ྜ≀ࡢ◊✲࡟᭷⏝࡛࠶ࡿࡇ࡜ࡀศ࠿ࡗ࡚

mgYb cm ࡛ࢫ࣌ࢡࢺࣝࢆ

cm–2 ࡢཌࡳ࡛

336

ᐃࡋࡓࢫ࣌ࢡࢺࣝࢆ㸪ᅗ 10 ࡟♧ࡋࡓ㸬࠸ࡿࡢ࡛㸪௒ᚋࡶ◊✲ࢆⓎᒎࡉࡏ࡚⾜ࡃணᐃ࡛࠶ࡿ㸬ࠉC ᆺ Yb2O3 ࡟ࡣ⤖ᬗᏛⓗ࡟ 2 ࢧ࢖ࢺᏑᅾࡋ㸪S3 ᑐ᭷ᶵ㔠ᒓ໬ྜ≀ࡢ◊✲࡜࠸࠺Ⅼ࠿ࡽࡣ㸪193Ir ࣓ࢫࣂ⛠ࡢ 8a ఩⨨࡟ Yb ࡢ 1/4 ࡀ㸪
C2 ᑐ⛠ࡢ 24d ఩⨨࡟ 3/4

࢘࢔࣮ࢫ࣌ࢡࢺࣝࡶ᭷⏝࡛࠶ࡿ㸬௒ᚋ 193Ir ࣓ࢫࣂࡀᏑᅾࡍࡿ㸬࣓ࢫࣂ࢘࢔࣮ࢫ࣌ࢡࢺ࡛ࣝࡣ㸪ࡇࢀࡽ࢘࢔࣮஧ࡘࡢࢧ࢖ࢺࡀ㆑ู࡛ࡁ࡚࠸ࡿ㸬ᖐᒓࡣᅄᴟ⤖ྜᐃࡀࡽ㸪◊✲ࢆⓎᒎࡉࡏ࡚⾜ࡃࡇ࡜ࢆィ⏬ࡋ࡚࠸ࡿ㸬ࡳ࡛

2ᐃࡀ࡛ࡁࡿࡼ࠺࡟ࡋ࡚㸪 197Au ࡜ే⏝ࡋ࡞–1

ᩘ e qQ = 10.8 mm s ࡢ྾཰ࡀ C3 ࢧ࢖ࢺ࡛㸪25.3 mm
155
Gd2O3 ࡶ Yb2O3 ࡜ྠᙧ࡛㸪Gd
s–1 ࡀ C2 ࢧ࢖ࢺ࡜࡞ࡿ㸬ᡂᯝࡢබ⾲ࢫ࣌ࢡࢺ࡛ࣝࡶ㸪஧ࡘࡢࢧ࢖ࢺࡀ᫂░࡟㆑ู࡛ࡁࡿ㸬

1. R. Cao, T. M. Anderson, P. M. B. Piccoli, A,. J.

2

–1

2

C3 ࢧ࢖ࢺࡣ e qQ = 10.85 mm s . C2 ࢧ࢖ࢺࡀ e qQ =–1

2

Schultz, T. F. Koetzie, Y. V. Geletii, E. Slonkina, B.

5.53 mm s ࡜ᖐᒓ࡛ࡁࡿ㸬e qQ ࡢ್ࢆࡶ࡜࡟㟁ሙ

Hedman, K. O. Hodgson, K. I. Hardcastle, X. Fang,໙㓄ࢆィ⟬ࡍࡿ࡜㸪Yb2O3 ࡛ࡣ C3 ࢧ࢖ࢺ 1.51022 V

M. L. Kirk, S. K. Knottenbelt, P. Kögerler, D,. G.

m–2㸪C2 ࢧ࢖ࢺ 3.41022 V m–2㸪Gd2O3 ࡛ࡣ C3㸪C2

Musaev, K. Morokuma, M. Takahashi, C. L. Hill, J.

ࢧ࢖ࢺࡣࡑࢀࡒࢀ 2.51022 ࠾ࡼࡧ 1.31022 V m–2

Am. Chem. Soc., 129, 11118 – 11133 (2007):࡜࡞ࡿ㸬඲⯡ⓗ࡟ Yb2O3 ࡢ࡯࠺ࡀ㟁ሙ໙㓄ࡀ኱ࡁࡃ

Terminal gold-oxo complexes- 318 -

3-2
㻥

JAEA-Review 2013-039

2. M. Sircoglou, S. Bontemps, M. Mercy, N. Saffon, M.

4. ῦ㤶㸪㧗ᶫ㸪᏷ᡞ㸪᪥ᮏ໬Ꮫ఍➨ 88 ᫓Ꮨᖺ఍Takahashi, G. Bouhadir, L. Maron, D. Bourissou,

㸦2008.3㸧ᮾி㸸࢖ࢵࢸࣝࣅ࣒࢘໬ྜ≀ࡢ 170Yb

Angew. Chem. Int. Ed., 46, 8583 – 8586 (2007):࣓ࢫࣂ࢘࢔࣮

ᐃ㸬

Transition-metal complexes featuring Z-type ligands:

5. 高橋，淺香，宍戸，第 45 回࢔࢖ࢯࢺ࣮ࣉ・放射n

線研究会（2008.7）東京：無機化合物の 170Yb メ

Agreement or discripancy between geometry and dconfiguration?

スバウアー測定．

3. J. Wang, M. Takahashi, T. Kitazawa, M. Takeda, J.

6. 高橋，今井，淺香，2008 日本放射化学会年会・

Rare Earth, 25, 647 (2007): Structure and bonding in

第 52 回放射化学討論会（2008.9）広島：Yb 酸

some Gd(III) metal complexes studied by three-

化物および塩化物の 170Yb メスバウアースペク

dimensional X-ray analysis and 155Gd Mössbauer

トル．

spectroscopy

7. 高橋，Mirzadeh, Bhargava, Bennett，2008 日本放4. M. A. Bennett, S. K. Bhargava, M. Takahashi, N.

射化学会年会・第 52 回放射化学討論会（2008.9）

Mirzadeh, S. H. Privér, Bull. Chem. Soc. Jpn., 82,

広島：三級ホスフィンを配位子とする二核金錯(2009), in press:

197

Au Mössbauer spectroscopic

studies of cyclometalated gold dimers containing 2-

体の 197Au メスバウアースペクトル
8. 高橋，平井，日本化学会第 89 春季年会（2009.3）

C6F4PPh2 ligands

船橋：ホスフィンオキシドを配位したランタノ
イド錯体の構造とメスバウアースペクトル．

ᅜ㝿఍㆟

9. 藤田，笹森，菊地，高橋，日本化学会第 89 春季

1. A Nakamura, A.F. Fuentes, Y. Okamoto, M.

年 会 （ 2009.3 ） 船 橋 ： 二 次 元 正 方 格 子 磁 性 体

Takahashi and M. Takeda, International Symposium

BBDTA·AuBr4 における磁気相転移

on the Industrial Applications of the Mössbauer

10. 高橋，根本，Mirzadeh, Bhargava, Bennett，第 46Effect, Budapest, Hungary, Aug. 2008: 151Eu- and回アイソトープ・放射線研究会（2009.7）東京：

155

Gd-Mössbauer Study of Defect-fluorite-type MO2-

ペルフルオロ基をもつ三級ホスフィンを配位し4+た有機金化合物の Au-197 メスバウアースペクト

LnO1.5 Solid Solutions (M=Ti, Hf, Zr, Ce, U, Th;

3+

Ln =Lanthanide)ル
11. 高橋，平井，2009 日本放射化学会年会・第 53

Ꮫ఍ㅮ₇回放射化学討論会（2009.9）東京：ホスフィン

1. 㧗ᶫ㸪ᮾ⯓㸪➉⏣㸪2006 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍࣭

オキシドを配位したランタニド(III)錯体の結晶➨ 50 ᅇᨺᑕ໬Ꮫウㄽ఍㸦2006.10㸧Ỉᡞ࣭ᮾᾏ㸸

構造と 151Eu および 155Gd メスバウアースペクト㸦ࢪࣁ࣮ࣟࣚࢻ㸧࣋ࣥࢮࣥ㢮ࡢ 127I ࣓ࢫࣂ࢘࢔

ル࣮ࢫ࣌ࢡࢺࣝ㸬12. 藤田，笹森，菊地，高橋，日本物理学会 2009 年

2. 綾部，㧗ᶫ，竹田，Costes，2006 日ᮏᨺᑕ໬学会年会・第 50 回放射化学討論会（2006.10）水戸・東海：Gd(III)を含む 3d−4f，4f−4f’系二核
錯体の

155

秋季大会（2009.9）熊本：有機磁性分子が作る二次元正方格子磁性体の基底状態

3-2

Gd メスバウアースペクトル．

3. ᫬⏣㸪⚟ᔱ㸪໭௦㸪➉⏣㸪Bhargava㸪日本化Ꮫ఍➨ 87 ᫓Ꮨᖺ఍㸦2007.3㸧྿⏣㸸trans㸫1,2-ࣅࢫ㸦ࢪࣇ࢙ࢽࣝ࣍ࢫࣇ࢕ࣀ㸧࢚ࢳࣞࣥࡀ㓄఩ࡋࡓ୕᰾㔠(I)㘒యࡢྜᡂ࡜ᵓ㐀࠾ࡼࡧ 31P NMR㸬- 319 -

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JAEA-Review 2013-039

3-3㺀࣐࢞ࣥ⥺ᦤືゅ┦㛵ἲࢆ⏝࠸ࡓ㔠ᒓࢱࣥࣃࢡ㉁άᛶ఩ࡢ㉸ᚤ⣽ሙᐃ㺁Measurement of Hyperfine Field of a Metal Site of Proteinby the Method of Perturbed Angular Correlation of Gamma-Rays
㔠ἑ኱Ꮫ ⌮ᕤ◊✲ᇦ ᶓᒣ᫂ᙪAkihiko Yokoyama, Institute of Science and Engineering, Kanazawa University࠙ࡣࡌࡵ࡟ࠚ
㏆ᖺࠊࢱࣥࣃࢡ㉁ࡢᵓ㐀࡜ᶵ⬟ࡢ㛵ಀࡀὀ┠ࡉࢀࠊ┒ࢇ࡟◊✲ࡀ⾜ࢃࢀ࡚࠸ࡿࠋ≉࡟⏕యศᏊ୰ࡢ㔠ᒓ࢖࢜ࣥࡣάᛶ୰ᚰ࡜ࡋ࡚㔜せ࡞ᙺ๭ࢆᢸ࠸ࠊࡑࡢᙺ
๭ࢆ⪃ᐹࡍࡿୖ࡛ pH ࡸ㓟໬㑏ඖ㟁఩࡞࡝ࡢ໬Ꮫⓗ⎔ቃ࡜㛵㐃ࡋࡓ≧ែࡢ᝟ሗࡣࠊ㠀ᖖ࡟㔜せ࡛࠶ࡿࠋ⌧ᅾࢱࣥࣃࢡ㉁ࡢᵓ㐀ࢆゎᯒࡍࡿࡓࡵࡢ୍⯡ⓗ࡞ᡭἲ࡛࠶ࡿ X ⥺ᵓ㐀ゎᯒ࡟ࡼࡗ࡚ࠊ⤖ᬗ໬ࡋࡓࢱࣥࣃ
ࢡ㉁ࡢヲ⣽࡞ᵓ㐀ࢆ ᐃ࡛ࡁࡿࠋࡋ࠿ࡋࠊᶵ⬟ࢆⓎ⌧ࡋ࡚࠸ࡿࡢࡣỈ⁐ᾮ୰࡛࠶ࡾࠊࢱࣥࣃࢡ㉁ࡢ⁐ᾮ୰࡛ࡢ≧ែ࡟㛵ࡍࡿ᝟ሗࡀᑡ࡞࠸ࠋȚ⥺ᦤື┦㛵
㸦PAC㸧ἲ࡛ࡣヨᩱࢆ⁐ᾮࡢࡲࡲ㸦in situ ᐃ㸧࡛ࡁࡿࡢ࡛ࠊᵓ㐀ࢆᦆ࡞࠺ࡇ࡜࡞ࡃࠊࡲࡓࡣᶵ⬟ࡀⓎ⌧࡛ࡁࡿ⎔ቃ࡟࠾࠸࡚㔠ᒓάᛶ㒊఩࿘㎶ࡢ㉸ᚤ⣽ሙࢆ ᐃ࡛ࡁࡿྍ⬟ᛶࡀ࠶ࡿࠋ ࡇࢀࡲ࡛࡟ሗ࿌ࡉࢀࡓ PAC ἲࡢ⏕యศᏊ࡬ࡢᛂ
⏝࡜ࡋ࡚ࡣࠊ௨ୗࡢࡼ࠺࡞౛ࡀ࠶ࡿࠋ㖡࢖࢜ࣥࢆྵ
ࡴࢱࣥࣃࢡ㉁ࡢ◊✲࡜ࡋ࡚ࠊ࢔ࢬࣜࣥࠊࣉࣛࢫࢺࢩ
࢔ࢽࣥ࡞࡝ࡢࣈ࣮ࣝ㖡ࢱࣥࣃࢡ㉁୰㔠ᒓ఩⨨࡟ࣉ࣮ࣟࣈぶ᰾ࢆᑟධࡍࡿࡇ࡜࡛ᦤືゅ┦㛵 ᐃࡀ࡞ࡉࢀ
ࡓࠋࡇࢀࡽࡢࢱࣥࣃࢡ㉁࡛ࡣ஧ࡘࡢ His ṧᇶ࡜ Cys
ṧᇶࠊMet ṧᇶࡢᅄࡘࡢ࢔࣑ࣀ㓟ṧᇶ࡟ࡼࡗ࡚㔠ᒓࡀᅖࡲࢀ࡚࠾ࡾࠊ๓ࡢ୕ࡘࡀ㔠ᒓ⤖ྜ࡟ᙉࡃ㛵୚ࡋࠊMet ࡣỈࡢ౵ධࢆ㜵࠸࡛㔠ᒓ఩ࡢᏳᐃᛶ࡟ᐤ୚ࡋ࡚
࠸ࡿࡇ࡜ࡀ ᐃ⤖ᯝ࠿ࡽㄽࡌࡽࢀࡓࠋࡑࡢ௚ࣉࣛࢫ
ࢺࢩ࢔ࢽࣥࡢ His ṧᇶࡢ୍ࡘࡀ஧ࡘࡢ His ṧᇶ࡜Cys ṧᇶࡢసࡿ㠃ෆ࡛㐠ືࡋ࡚࠸ࡿࡇ࡜ࡀ PAC ࢫ࣌ࢡࢺࣝ࡟཯ᫎࡉࢀࠊືⓗ࡞᝟ሗ࡟ࡘ࠸࡚ࡶᚓࡽࢀ
࡚࠸ࡿࠋ௚࡟ࡶ㖡ࢱࣥࣃࢡ㉁࡛ࡣ」ᩘࡢ㖡࢖࢜ࣥࢆྵࡴࣛࢵ࣮࢝ࢮ࡞࡝ࡢ࣐ࣝࢳ㖡ࢱࣥࣃࢡ㉁ࡢ ᐃ౛ࡀ࠶ࡾࠊ㖡௨እ࡛ࡶள㖄࢖࢜ࣥࢆྵࡴࢱࣥࣃࢡ㉁ࡢ
◊✲ࡸࠊ࣐࢘ࢫࢆ౑ࡗࡓ in-vivo ࡛ࡢ ᐃ౛ࡶ࠶ࡿࠋ
ࡇࢀࡽࡢ◊✲ࡢከࡃࡣ⏕య୰ࡢ໬ྜ≀࡟ࡘ࠸࡚㔠ᒓඖ⣲ࡢᙺ๭ࢆ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࢆ┠ᣦࡋ࡚࠸ࡿࠋ ⚾ࡢ◊✲ࢢ࣮ࣝࣉ࡛ࡣࠊࡇࢀࡲ࡛࡟άᛶ୰ᚰ࡟㖡ࢧ࢖ࢺࢆᣢࡘ㔠ᒓࢱࣥࣃࢡ㉁࣐ࣅࢩ࢔ࢽࣥࡢ㔝⏕ᆺࡸኚ␗య(15 ఩ࡢ Thr ࢆ Ala ࡟⨨ࡁ᥮࠼ࡓࡶࡢ)ࡢ⁐ᾮ୰ࡢ≧ែ࡟ࡘ࠸࡚ࡢ᝟ሗࢆᚓࡿࡇ࡜ࢆ┠ⓗ࡜ࡋ࡚ࠊ࣐ࣅࢩ࢔ࢽࣥࡢάᛶ୰ᚰ࡛ࡢ㉸ᚤ⣽ሙ ᐃࢆ PAC
ἲ࡛ヨࡳࡓࠋࡇࡢ◊✲࡟࠾࠸࡚኱⭠⳦࡟ࡼࡾ⏕ྜᡂࡋࡓ࣐ࣅࢩ࢔ࢽࣥࡢ㖡ࢆ PAC ࣉ࣮ࣟࣈぶ᰾ 117Cd
㸦ń117In, T1/2=2.49 h㸧࡟⨨᥮ࡋࠊ㔝⏕ᆺ࡜ኚ␗ᆺ
ࡑࢀࡒࢀࡢ㖡άᛶ㒊఩࡟࠾ࡅࡿ㉸ᚤ⣽ሙ࡟㐪࠸ࡀ࠶ࡿࡇ࡜ࢆぢฟࡋࡓࠋ[1,2] ࡲࡓࠊࡇࡢ ᐃ࠿ࡽᚓࡽ
ࢀࡓ᝟ሗࢆࡼࡾヲࡋࡃ㆟ㄽࡍࡿࡓࡵ࡟ࠊ㓄఩ඖ⣲ࡸ㓄఩ᩘࡀ㢮ఝࡋࡓ㘒య࡛ࡢ㉸ᚤ⣽ሙ ᐃࢆ 117Cd ࡢ࡯࠿࡟ 111In㸦ń111Cd, T1/2=2.80 d㸧ࡸ 111mCd㸦ń111Cd,
T1/2=48.5 min㸧࡞࡝ࡢ PAC ぶ᰾✀ࢆ⏝࠸࡚⾜ࡗࡓࠋ
[3]ࡋ࠿ࡋࠊࡇࢀࡽࡢ᰾✀ࡣ༙ῶᮇࡀ▷ࡃࠊ⤫ィࡢⰋ࠸ࢹ࣮ࢱࢆྲྀࡿࡇ࡜ࡀ㞴ࡋ࠸ࠊࡲࡓ▷᫬㛫࡛ヨᩱࢆసᡂࡋ࡞ࡅࢀࡤ࡞ࡽ࡞࠸࡜࠸ࡗࡓၥ㢟ࡀ࠶ࡗࡓࠋ
ࡑࡇ࡛ᮏ◊✲࡛ࡣ㔠ᒓࢱࣥࣃࢡ㉁࡟ྲྀࡾ㎸ࡴ
PAC ᰾✀࡟ࠊẚ㍑ⓗ༙ῶᮇࡢ㛗࠸ 111Ag(ń111Cd,
T1/2=7.45 d)ࢆ⏝࠸࡚⤫ィࡢⰋ࠸ࢹ࣮ࢱࢆᚓࡿࡇ࡜
ࢆ┠ⓗ࡜ࡋࡓࠋ111Ag ࡢቯኚ⏕ᡂ≀࡛࠶ࡿ 111Cd ࡢ㓟໬ᩘࡣ㖡࡜ྠࡌ+2 ࡛࠶ࡿࡓࡵࠊࡇࡢ᰾✀ࢆ⏝࠸ࡿࡇ࡜࡛⨨᥮๓ࡢ㖡άᛶ㒊఩࡟ࡼࡾ㏆࠸໬Ꮫ≧ែ࡛ ᐃࢆ⾜࠼ࡿ࡜࠸࠺฼Ⅼࡶᮇᚅ࡛ࡁࡿࠋཎᏊ⅔࡛ࡢ୰ᛶᏊ↷ᑕ࡛ PAC ぶ᰾✀࡛࠶ࡿ 111Ag ࢆ〇㐀ࡋࠊ ᐃ࡟㐺ࡋࡓࢺ࣮ࣞࢧ࣮⁐ᾮࢆㄪᩚࡍࡿᡭἲࢆ☜❧ࡋࠊࡇࢀࢆ⏝࠸࡚✀ࠎࡢ㖟㘒య࡜ࢱࣥࣃࢡ㉁ヨᩱࡢ㟁ሙ໙㓄್ࢆ ᐃࡍࡿࡇ࡜ࢆヨࡳࡓࠋ࠙ࣉ࣮ࣟࣈ᰾ࡢ〇㐀ࠚ
111Ag ࡢ〇㐀ࡣࠊᕷ㈍ࡢኳ↛ྠ఩య⤌ᡂࡢ Pd ⟩㸦⣙2.55 g㸧ࢆ⏝࠸࡚ཎᏊຊ◊✲㛤ⓎᶵᵓཎᏊຊ⛉Ꮫ◊✲ᡤ JRR-3㸦ࡲࡓࡣ JRR-4㸧ཎᏊ⅔୰࡟㏦ධࡋࠊ⇕୰ᛶᏊ↷ᑕࢆ 20 ศ㛫⾜ࡗࡓࠋࡑࡢᚋ Pd ⟩ࢆ 5 ᪥㛫ᨺ⨨ࡋࠊ110Pd(n,Ǆ)111Pd ཯ᛂ(཯ᛂ᩿㠃✚ 0.70 b)࡟
ࡼࡗ࡚⏕ࡌࡓ 111Pd (T1/2=23.4 min)ࢆ඘ศ࡟ ǃ㸫ቯኚ
ࡉࡏ࡚ 111Ag(⣙ 60MBq)ࢆ〇㐀ࡍࡿ࡜࡜ࡶ࡟↷ᑕ᫬࡟⏕ᡂࡍࡿ๪⏕ᡂ≀ࢆῶ⾶ࡉࡏࡓࠋᅗ㸯࡟ᨺ⨨ᚋࡢ↷ᑕヨᩱ࡟ࡘ࠸࡚ࠊGe ༙ᑟయ᳨ฟჾࢆ⏝࠸ࡓ࣐࢞ࣥ
⥺ࢫ࣌ࢡࢺࣝࡢ୍౛ࢆ♧ࡋࡓࠋ㹙4㹛

JRR-3M ࠾ࡼࡧ JRR-4 Ẽ㏦⟶ࠊ᰾≀ᛶ

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JAEA-Review 2013-039

Counts/channel

10 4
Au-198

10 3
Ag-111

10 2

Br-82
Pd-10910 1
Ir-192

10

0

0

200

400
600
Energy/keV

800

1000

ᅗ㸯㸬↷ᑕヨᩱࡢȚ⥺ࢫ࣌ࢡࢺࣝࡢ୍౛ࠋ
୺࡞Ț⥺ࡣ┠ⓗࡢ 111Ag ࡛࠶ࡿࡇ࡜ࡀࢃ࠿ࡿࠋࡑࡢ௚ ࡣ ࢱ࣮ ࢤࢵ ࢺ ୙⣧ ≀㉳ ※ ࡢࡶ ࡢ࡜ ࠊ ๪⏕ ᡂ≀
㸦109Pd, T1/2=13.43 h㸧ࡀࢃࡎ࠿࡟☜ㄆ࡛ࡁࡿࠋ
࠙ヨᩱㄪ〇ࠚ
ୖグࡢ↷ᑕヨᩱࢆி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤ࡟㐠ᦙࡋࠊୗグࡢ㸰ࡘࡢࢫ࣮࣒࢟࡟ᚑࡗ࡚ 111Ag ࢆ↷ᑕヨᩱ࠿ࡽศ㞳ࡋ࡚ࢺ࣮ࣞࢧ࣮⁐ᾮ࡜ࡋࡓࠋ㖟㘒యヨᩱࡣࢫ࣮࣒࢟㸯ࢆ᥇⏝ࡋࠊࢱࣥࣃࢡ㉁ヨᩱࡣึᮇ࡟ࡣࢫ࢟
࣮࣒㸯ࢆࠊᚋ࡟ࢫ࣮࣒࢟㸰ࢆ᥇⏝ࡋࡓࠋࢫ࣮࣒࢟㸯↷ᑕࡋࡓ Pd ⟩ 1 ᯛ࡟ࡘࡁ⋤Ỉࢆ 2 mL ຍ࠼ࠊ࣍ࢵࢺࣉ࣮ࣞࢺୖ࡛ຍ⇕ࡋ࡚⁐ゎࡋࡓࠋᢸయ࡜ࡋ࡚◪㓟㖟ࢆ 40 mg ຍ࠼ࠊỈࢆຍ࠼࡚⣙ 50ml ࡟ࡋࡓࠋ⏕ᡂࡋࡓⓑⰍࡢ AgCl ỿẊࢆ㐲ᚰศ㞳(3000 rpmࠊ5min)࡛ྲྀࡾศࡅࠊୖ⃈ࡳࡣูࡅ࡚࠾࠸ࡓࠋࡇࡢỿẊ࡟࢔ࣥࣔࢽ࢔Ỉ 6 mL ࢆຍ࠼࡚ຍ⇕ࡋ࡚⁐ゎࡋࠊ⃰ሷ㓟ᩘ⁲ࠊ⃰◪㓟 4 mL ࢆຍ࠼࡚෌ࡧ AgCl ỿẊࢆ⏕ᡂࡉࡏࡓࠋࡇࡢỿẊࢆ㐲ᚰศ㞳࡛ྲྀࡾศࡅࠊ6M
NaOH ࢆ 5mL ຍ࠼࡚‫‮‬ᾎ࡛⣙ 30 ศຍ⇕ࡍࡿ࡜ỿẊࡀ㯮⥳Ⰽࡢ Ag2O ࡟࡞ࡗࡓࠋࡑࡢᚋ㐲ᚰศ㞳࡛ࡇࡢỿẊࢆྲྀࡾศࡅ࡚⃰◪㓟 5 mL ࡛⁐࠿ࡋ࡚ࢺ࣮ࣞࢧ
࣮⁐ᾮ࡜ࡋࡓࠋヨᩱࡢᨺᑕ⬟ࡀᑡ࡞࠸ሙྜࡣࠊ1 ᅇ┠ࡢ㐲ᚰศ㞳ู࡛ࡅ࡚࠾࠸ࡓୖ⃈ࡳ࡟ྠᵝࡢ᧯సࢆ⾜ࡗ࡚ᨺᑕ⬟ᡂศࡢศ㞳ࢆ㐺ᐅ⾜ࡗࡓࠋࢫ࣮࣒࢟㸰ヨᩱࢆࣅ࣮࣮࢝࡟⛣ࡋ᥮࠼࡚ Pd ⟩ 1 ᯛ࡟ࡘࡁ⋤Ỉ 2 mL ࢆຍ࠼ࠊ࣍ࢵࢺࣉ࣮ࣞࢺୖ࡛ຍ⇕ࡋ࡚᏶඲࡟⁐ゎࡉࡏࡓࠋ㝜࢖࢜ࣥ஺᥮ᶞ⬡㸦Dowex 1 × 8
100-200 mesh㸧ࢆ࣒࢝ࣛ
㸦BIO-RAD ♫ࠊᐜ㔞 20 mL㸧࡟඘ሸࡋ࡚⃰ሷ㓟࡛ࢥࣥࢹ࢕ࢩࣙࢽࣥࢢࡋࠊヨᩱ⁐ᾮࢆὶࡋࡓࠋࡑࡢᚋࠊࡲࡎ⃰ሷ㓟 10 mL ࢆὶࡋ࡚◚Რࡋࠊḟ࠸࡛⃰ሷ㓟 20 mL ࢆὶࡋ࡚ࡇࢀࢆศྲྀࡋࡓࠋ
඲࡚ࡢ࣒࢝ࣛ࠿ࡽศྲྀࡋࡓ⁐ฟᾮࢆ 1 ࡘ࡟ࡲ࡜ࡵࠊ
࣍ࢵࢺࣉ࣮ࣞࢺ࡛⣙ 3 mL ࡲ࡛ຍ⇕⃰⦰ࡋࠊ6M

NaOH ࡛ pH 7 ࡟ㄪ〇ࡋࡓᚋ࡟෌ࡧ⣙ 2 mL ࡟࡞ࡿࡲ࡛ຍ⇕⃰⦰ࡋࠊࡇࢀࢆ 111Ag ࡢࢺ࣮ࣞࢧ࣮⁐ᾮ࡜ࡋࡓࠋ ࢱࣥࣃࢡ㉁ヨᩱࡢㄪᩚ࡟࠾࠸࡚ࡣࠊసᡂࡋࡓࢺࣞ
࣮ࢧ࣮⁐ᾮࢆ 6M NaOH ࡛୰࿴ࡋࠊ⏕ྜᡂࡋࡓ࣐ࣅ
ࢩ࢔ࢽࣥ⁐ᾮ㸦200ǍM㸧ࢆຍ࠼ 6 ᫬㛫࠿ࡽ୍ᬌᨩᢾ
ࡋ࡚ 111Ag ࢆྲྀࡾ㎸ࡲࡏࡓࠋࡑࡢᚋ HEPES ⦆⾪ᾮࢆ⏝࠸࡚ pH 7.5 ࡟ㄪᩚࡋࡓ Sephadex G25 ࣒࡛࢝ࣛࠊࢱࣥࣃࢡ㉁࡟ྲྀࡾ㎸ࡲࢀ࡞࠿ࡗࡓవศ࡞ 111Ag
ࢆ㝖࠸ࡓᚋࠊ⢓ᛶࢆ㧗ࡵ࡚ࢱࣥࣃࢡ㉁ࡢᣑᩓ㐠ືࢆᢚ࠼ࡿࡓࡵ࡟ࢫࢡ࣮ࣟࢫࢆ⤊⃰ᗘ 50%࡟࡞ࡿࡼ࠺
ຍ࠼࡚ࠊ ᐃࡢ㝿࡟ࡣࢱࣥࣃࢡ㉁ࡢኚᛶࢆ㜵ࡄࡓࡵ࣌ࣝࢳ࢚⣲Ꮚࡢୖ࡛෭ࡸࡋ࡞ࡀࡽ⾜ࡗࡓࠋ㖟㘒యヨᩱ࡟ࡘ࠸࡚ࡣࠊసᡂࡋࡓࢺ࣮ࣞࢧ࣮⁐ᾮ࡟ྛ✀࣮࢟ࣞࢺ๣㸦o-phenanthrolineࠊbismuthiolࠊ࢜࢟ࢩࣥࠊDDCࠊBPHAࠊ࢟ࢼࣝࢪࣥ㓟㸧ࢆຍ࠼࡚㘒యヨᩱࢆㄪ〇ࡋࡓࠋ࠙PAC ᐃࠚ
㸰ᮏࡢ࢝ࢫࢣ࣮ࢻȚ⥺ࡢゅᗘ┦㛵ࢆㄪ࡭ࡿࡓࡵࠊ
㸲ࡘࡢ᳨ฟჾࢆ 0rࠊ 90rࠊ180rࠊ270r᪉ྥ࡟
タ⨨ࡋࠊ᫬㛫ᚤศᆺ PAC ᐃἲ࡛ィ ࡋࡓࠋ᳨ฟ
ჾ࡟ࡣ᫬㛫ศゎ⬟࡟ඃࢀࡓ BaF2 ࢩࣥࢳ࣮ࣞࢱࢆ౑
⏝ࡋࡓࠋ
111Ag ࢆぶ᰾࡜ࡋ࡚⏝࠸ࡓ࡜ࡁ࡟ࠊ
㟁ሙ໙㓄ࡢࡳࢆ
ᦤື࡜ࡋ࡚⪃࠼ࡓሙྜࡢᦤືಀᩘ A22G22(t)ࡣ௨ୗ
ࡢࡼ࠺࡟࡞ࡿࠋ  

A22G22(t) A22^S0  S1 cos(6ZQC1t)  S2 cos(6ZQC2t)  S3 cos(6ZQC3t)` 㸦㸯㸧
ࡇࡇ࡛ࠊSn,Cn ࡣ㠀ᑐ⛠ࣃ࣓࣮ࣛࢱȞ࡟ࡼࡗ࡚୚࠼
ࡽࢀࠊȞ=0 ࡢሙྜࠊ
  
10
5
A22 ­ 13½
A22G22 (t )®1  cos(6ZQt )  cos(12ZQt )  cos(18ZQt )¾
5 ¯ 7
7
7
¿
 㸦㸰㸧
࡜࡞ࡿࠋ
ᐇ㦂࡛ᚓࡽࢀࡓ TDPAC ࢫ࣌ࢡࢺࣝ࡟ 㸯 ᘧࢆࣇ࢕ࢵࢸ࢕ࣥࢢࡍࢀࡤࠊ㟁Ẽᅄ㔜ᴟ࿘ἼᩘȰ4 ࠾ࡼࡧ
111
Cd ࣉ࣮ࣟࣈ᰾఩⨨࡛ࡢ㟁ሙ໙㓄ࢆồࡵࡿࡇ࡜ࡀ
࡛ࡁࡿࠋࡓࡔࡋࠊȰ4 ࡣࢫ࣌ࢡࢺࣝ࡟ࡼࡗ࡚ Gaussศᕸࡢศᩓࢆ௬ᐃࡋࡓࠋ ᐃࡉࢀࡓ࣐ࣅࢩ࢔ࢽࣥ࡟
ᑐࡍࡿᐊ ௜㏆࡛ ᐃࡋࡓ TDPAC ࢫ࣌ࢡࢺࣝࡢ౛
ࢆ㖟㘒యࡢࢹ࣮ࢱ࡜ඹ࡟ᅗ 2 ࡟♧ࡍࠋ⤫ィⓗ࡟࠶ࡿ⛬ᗘ‶㊊࡛ࡁࡿࢫ࣌ࢡࢺࣝࢆᚓࡿࡇ
࡜࡟ᡂຌࡋࡓ o-phenanthroline㘒య㸦ᅗ2a㸧࡜bismuthiol㘒య㸦ᅗ2b㸧࡜ẚ㍑ࡍࡿ࡜ࠊ࣐ࣅࢩ࢔ࢽ

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JAEA-Review 2013-039

ࣥ㸦ᅗ2c㸧࡟ࡘ࠸࡚ࡣAg࢖࢜ࣥࡢࢱࣥࣃࢡ㉁࡬ࡢྲྀ
ࡾ㎸ࡳ⋡ࡀᝏ࠸ࡓࡵヨᩱࡢᨺᑕ⬟ࡀᙅࡃࠊ࠶ࡲࡾ⤫ィࡢⰋ࠸ࢹ࣮ࢱࢆᚓࡿࡇ࡜ࡀ࡛ࡁ࡞࠿ࡗࡓࡀࠊఱ࡜
࠿ࣇ࢕ࢵࢸ࢕ࣥࢢྍ⬟࡞ணഛⓗ࡞㹎㸿㹁ࢫ࣌ࢡࢺࣝࢆ ᐃ࡛ࡁࡓࠋ㹙㹛


(a)


A22G22 (t)A22G22 (t)A22G22 (t)







t/ns

(b)







t/ns

(c)







t/ns

ᅗ㸰㸬᫬㛫ᚤศ㹎㸿㹁ࢫ࣌ࢡࢺࣝࡢ౛ࠋ
࠙⤖ㄽࠚ ↷ᑕࡋࡓ Pd ⟩ࡼࡾ 111Ag ࢆྲྀࡾฟࡋ࡚ࢺ࣮ࣞࢧ
࣮⁐ᾮࢆసᡂࡋࠊ⏕యヨᩱ➼࡟ᑐࡋ࡚ PAC ᐃࢆ⾜࠺ࡇ࡜࡟ᡂຌࡋࡓࠋࡓࡔࡋࠊ௒ᅇࡢᐇ㦂࡛ ᐃࡋࡓ
ࢱࣥࣃࢡ㉁ヨᩱࡣᨺᑕ⬟ࡀᙅࡃࠊ⤫ィࡢⰋ࠸ࢹ࣮ࢱ
ࢆྲྀࡿࡇ࡜ࡀฟ᮶࡞࠿ࡗࡓࠋࡓࡔࡋࠊࡇࢀࡲ࡛࡟ࢫ
࣮࣒࢟㸰࡟ࡼࡗ࡚↓ᢸయࡢ 111Ag ࢺ࣮ࣞࢧ࣮ࡢసᡂ
ᡭἲࢆ☜❧࡛ࡁࡓࡢ࡛ࠊࡇࢀ࠿ࡽᨺᑕ⬟ࢆቑ㔞ࡍࢀࡤឤᗘࡢⰋ࠸ᐇ㦂ࢆ⾜࠺ࡇ࡜ࡀᮇᚅ࡛ࡁࡿࠋ
ࣇ࢕ࢵࢸࣥࢢ࡟ࡼࡗ࡚ồࡵࡽࢀࡓᅄ㔜ᴟ࿘ἼᩘǚQ 㟁ሙ໙㓄ࡣୗグࡢࡼ࠺࡟㟁Ẽᅄ㔜ᴟ࣮࣓ࣔࣥࢺ
㹏ࠊࢫࣆࣥ㔞Ꮚᩘ㹇ࠊ࡜㠀ᑐ⛠ࣃ࣓࣮ࣛࢱ ǈ ࡛♧ࡉ
ࢀࡿࠋ

ZQ



eQVzz
4 I (2 I  1)!

ࡇࡢᘧࢆ౑ࡗ࡚ࠊ⌧᫬Ⅼࡲ࡛࡛ᚓࡽࢀ࡚࠸ࡿࢫ࣌ࢡ
ࢺࣝ࡟ࡘ࠸࡚ࠊ㟁ሙ໙㓄ࢆ⟬ฟࡋࡓࠋ
㹙6㹛௒ᅇ 111Ag
࡛ ᐃࡉ ࢀࡓ 㟁 ሙ໙ 㓄ࢆ ࠊ ௨๓ ࡟ู ࡢ ࣉࣟ ࣮ࣈ
㸦111Inࠊ111mCd㸧ࢆ⏝࠸࡚ ᐃࡉࢀࡓࢹ࣮ࢱ࡜ẚ㍑
ࡍࡿ࡜ࠊ࢜࢟ࢩࣥ㘒య࡛ࡣࣉ࣮ࣟࣈ᰾ࡀྠࡌ 111Cdࡢ୰㛫‽఩࡟ቯኚࡍࡿ 111Inࠊ111mCd ࡜ẚ㍑ࡋ࡚஧ಸ௨ୖ኱ࡁࡃ࡞ࡗ࡚࠸ࡿࠋDDC ࡛ࡣẚ㍑ⓗ㏆࠸್࡜࡞ࡗ࡚࠸ࡿࡶࡢࡢࠊBPHA ࡛ࡶ࢜࢟ࢩࣥ࡜ྠᵝࠊ111Ag
ࡢ᪉ࡢ್ࡀ኱ࡁࡃ࡞ࡗ࡚࠸ࡿࠋ඲యⓗ࡟ 111Ag ࢆ⏝࠸ࡿࡇ࡜࡟ࡼࡾヨᩱ࡛ࡣ㟁ሙ໙㓄್ࡀ኱ࡁࡃ࡞ࡿഴ
ྥࡀࡳ࠼ࡿࠋ࢜࢟ࢩࣥࠊDDCࠊBPHA ࡣㄗᕪࡀ኱ࡁ
࠸ࡢ࡛ㄗᕪ⠊ᅖෆ୍࡛⮴ࡋ࡚࠸ࡿྍ⬟ᛶࡀ࠶ࡿࡀࠊ
ẚ㍑ⓗ⤫ィࡢⰋ࠸࢟ࢼࣝࢪࣥ㓟࡛ࡣࠊ᫂ࡽ࠿࡟ 111Ag
ࡢࢹ࣮ࢱࡣ኱ࡁ࡞್ࢆ♧ࡋ࡚࠸ࡿࠋ୍᪉ࠊ⏕యヨᩱ࡛࠶ࡿ࣐ࣅࢩ࢔ࢽ࡛ࣥࡣࠊࡇࡕࡽࡶ࢚࣮ࣛࡀ኱ࡁ࠸
ࡀࠊ㏫࡟ 111Ag ࡢࢹ࣮ࢱࡢ᪉ࡀᑠࡉ࠸ࠋࡇ࠺࠸ࡗࡓࠊ
ࣉ࣮ࣟࣈぶ᰾࡟ࡼࡿ㟁ሙ໙㓄್ࡢ㐪࠸ࡣࠊࣉ࣮ࣟࣈ
ぶ᰾ࡢቯኚࡢᚋ㑇ຠᯝࡢྍ⬟ᛶࡀ࠶ࡿࠋࣉ࣮ࣟࣈ᰾
ࡀྠࡌ 111Cd ࡛࠶ࡿ୕ࡘࡢࣉ࣮ࣟࣈぶ᰾ࡢቯኚࡣࠊ
111mCd ࡣ᰾␗ᛶయ㌿⛣ࠊ111In ࡣ EC ቯኚࠊ111Ag ࡣǃ㸫ቯኚ࡜ࠊ୕ࡘ࡜ࡶ␗࡞ࡗࡓቯኚ࡛࠶ࡿࠋࡇࡢຠᯝ
࡟ࡘ࠸࡚ࡶ㠀ᖖ࡟⯆࿡῝࠸ࡢ࡛ࠊࡇࢀ࠿ࡽ᳨ウࡋ࡚࠸ࡁࡓ࠸ࠋ࠙ཧ⪃ᩥ⊩ࠚ
[1] ᶫᮏ▱඾ࠊᶓᒣ᫂ᙪࠊ∦ᒸ㑥㔜ࠊ㧗⏣┿⏤Ꮚࠊ⳥Ọⱥᑑࠊᮌୗဴ୍ࠊᮧୖᖾᘯࠊ㧗ᐑᖾ୍ࠊ኱ஂಖ
჆㧗ࠊKURRI-KR-118, pp.62-65 (2005).
[2] A. Yokoyama, T. Hashimoto, K. Ihara, H.
Kikunaga, N. Kinoshita, I. Yamazaki, K.
Kataoka, M. Yanase, M. Takata, Y. Murakami,
K. Takamiya, M. Tanigaki and Y. Ohkubo,
Hyperfine Int., 181, 69-73 (2008).
[3]ᶓᒣ᫂ᙪࠊᶫᮏ▱඾ࠊ∦ᒸ㑥㔜ࠊ⳥Ọⱥᑑࠊᮌୗ
ဴ୍ࠊᮧୖᖾᘯࠊ㧗ᐑᖾ୍ࠊ኱ஂಖ჆㧗ࠊబ⸨ ΅ࠊᩪ⸨ ┤ࠊKURRI-KR(CD)-6, pp.41-45 (2006).
[4] ᶓᒣ᫂ᙪࠊᒣ㷂㐓㑻ࠊᮧୖᖾᘯࠊ኱ஂಖ჆㧗ࠊబ⸨ ΅ࠊKURRI-KR(CD)-10, pp.33-36 (2007).
[5] ᶓᒣ᫂ᙪࠊᒣ㷂㐓㑻ࠊ㕥ᮌ኱௓ࠊ∦ᒸ㑥㔜ࠊ㧗ᐑᖾ୍ࠊ኱ஂಖ჆㧗ࠊబ⸨΅ࠊ
KURRI-KR(CD)-136, pp.39-42 (2008).
[6] ᒣ㷂㐓㑻ࠊすᑿṇᶞࠊ∦ᒸ㑥㔜ࠊᶓᒣ᫂ᙪࠊబ⸨ ΅ࠊ㧗ᐑᖾ୍ࠊ኱ஂಖ჆㧗ࠊ
KURRI-KR(CD) in press (2009).

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࠙ᡂᯝࡢබ⾲ࠚ㸬ᶓᒣ᫂ᙪࠊᒣ㷂㐓㑻ࠊᮧୖᖾᘯࠊ
኱ஂಖ჆㧗ࠊబ⸨΅ࠊ
ࠕ3$& ἲࢆ฼⏝ࡋࡓ⏕యศᏊάᛶ఩࡟࠾ࡅࡿ
㉸ᚤ⣽ሙ ᐃ̿$J ࢆ⏝࠸ࡓ 3$& ᐃࠖࠊி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤᑓ㛛◊✲఍ሗ࿌᭩.855,.5 &' SS  㸬ᶓᒣ᫂ᙪࠊᒣ㷂㐓㑻ࠊ㕥ᮌ኱௓ࠊ
∦ᒸ㑥㔜ࠊ㧗ᐑᖾ୍ࠊ኱ஂಖ჆㧗ࠊబ⸨΅ࠊࠕ$J ࢆ⏝࠸ࡓ 3$& ἲ࡟ࡼࡿ࣐ࣅࢩ࢔ࢽࣥࡢ
㉸ᚤ⣽ሙ ᐃࠖࠊி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤᑓ㛛◊✲఍ሗ࿌᭩ .855,.5 &' SS 
㸬ᒣ㷂㐓㑻ࠊすᑿṇᶞࠊ∦ᒸ㑥㔜ࠊᶓᒣ᫂ᙪࠊబ⸨΅ࠊ㧗ᐑᖾ୍ࠊ኱ஂಖ჆㧗ࠊࠕぶ᰾ࣉ࣮ࣟࣈ $J ࢆ⏝࠸ࡓ 3$& ᐃࠖࠊி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤᑓ㛛◊✲఍ሗ࿌᭩.855,.5 &' LQSUHVV  3-3- 323 -

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JAEA-Review 2013-039

3-4ప᰾೫ᴟ࡟ࡼࡿᙉ☢ᛶయࡢෆ㒊☢ሙࡢ⢭ᐦᐃStudy of Hyperfine Field using Low-temperature Nuclear Orientation኱▮ 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᪂₲኱Ꮫ࢔࢖ࢯࢺ࣮ࣉ⥲ྜࢭࣥࢱ࣮

Radioisotope Center, Niigata University㸯㸰㧗࢚ࢿࣝࢠ࣮ຍ㏿ჾ◊✲ᶵᵓ୰ᛶᏊ◊✲ᡤ
Neutron Science Laboratory, KEK㸰㸱ᐩᒣ኱ᏛᕤᏛ㒊㸱

Faculty of Engineering, Toyama Universityࡗ࠿ࡅ࡟࡞ࡗࡓࡢࡣ㸪ᪧ཭ࡢ 1-6WRQH ࠿㸯㸬ࡣࡌࡵ࡟
ࡇࢀࡲ࡛ᡃࠎࡣ㸪㉸ప᰾ᩚิ⿦⨨ࢆ⏝࠸ࡽ &(51,62/'( ࡛ࡢ +I ࡢ +LJK6SLQ,VRPHU࡚ከࡃࡢཎᏊ᰾ࡢ㉸ᚤ⣽┦஫స⏝ࡢ◊✲ࢆ⾜ࡢ☢Ẽ࣮࣓ࣔࣥࢺࢆ

ᐃࡍࡿィ⏬ࡀᥦ᱌ࡉࢀ

ࡗ࡚ࡁࡓࠋࡇࡢሙྜ㉸ᚤ⣽┦஫స⏝ࡢ኱ࡁࡉࡇ࡜࡟ጞࡲࡿࠋ+I ࡢ㕲୰ࡢෆ㒊☢ሙࡣᡃࠎࡀ

ࡣཎᏊ᰾ࡢ㹥ᅉᏊ࡜ෆ㒊ሙࡢ✚࡟࡞ࡿࠋࡋࡓ

+I ࡢ㕲୰ࡢඹ㬆ほ ᡂຌࡋ࡚࠸ࡓࠕ㸯ࠖࠋࡀࡗ࡚ཎᏊ᰾ࡢ☢Ẽ࣮࣓ࣔࣥࢺࡀ▱ࡽࢀ࡚࠸ᐇ㦂ࡣ  ᖺ㸶᭶࡟ &(51,62/'( ࡛⾜ࢃࡿ࡜ࡁࡣ㸪ࡇࡢ㉸ᚤ⣽┦஫స⏝࠿ࡽෆ㒊☢ሙࢀࡓࠋ᪥ᮏ࠿ࡽࡣ⚾௨እ࡟኱ᆤ㸦᪂₲኱㸧ࠊすࢆ⢭ᗘࡼࡃồࡵࡿࡇ࡜ࡀฟ᮶ࡿࡋ㸪㏫࡟ෆ㒊ᮧ㸦ᐩᒣ኱㸧ࠊṊ⸨㸦.(.㸧➼ࡀཧຍࡋࡓࠋᬑ

☢ሙࡀ▱ࡽࢀ࡚࠸ࡿ࡜ࡁࡣཎᏊ᰾ࡢ㹥ᅉᏊࢆ

㏻ࡣỴᐃ࡛ࡁࡿࠋࡲࡓᐇ㝿ࡢᐇ㦂࡛ࡣపࡃ౑ࢃࢀࡿࡀࠊࡇࡢ◊✲࡛ࡣ࣐࣮࢞ࣥ⥺ࡢ␗࡛ࡢᗘィ࡜ࡋ࡚ &R)H ࠶ࡿ࠸ࡣ &R)H ࡀⰋ

ᗘィ࡜ࡋ࡚ෆ㒊☢ሙ࡜ཎᏊ᰾ࡢ☢Ẽ࣮࣓ࣔࣥ᪉ᛶࡀ኱ኚ኱ࡁ࠸ࡢ࡛㸪ࢺࡀࡍ࡛࡟Ⰻࡃ▱ࡽࢀࡓࡶࡢࢆ⏝࠸ࡿࠋᬑ㏻

ឤᗘࡢ࠶ࡿࡶࡢࡀᚲせ࡛࠶ࡿࠋ

ࡣ &R ࡢ༢⤖ᬗ୰ࡢ &R࠶ࡿ࠸ࡣ㕲୰ࡢ &R࠾ࡼࡧ &R ࡞࡝ࡀ௦⾲ⓗ࡟⏝࠸ࡽࢀࡿࠋ
௒ᅇ㸪ࡑࡇ࡛༙ῶᮇ  ᪥ࡢ ,U)H ࢆᮾᾏࡢཎ
Ꮚ⅔ࢆ⏝࠸࡚సࡾࠊ

ᗘࡢ㧗࠸࡜ࡇࢁ࡛⏝࠸ࡿ㕲୰ࡢ,U) ࡜ &R ࡢ༢⤖ᬗࡣ㧗౯࡛࠶ࡿࡢ࡛ )FF ࡢᗘࡀ㧗࠸࡜ࡁ࡟ࠊ

ᗘィ࡜ࡋ࡚᪥ᮏ࠿ࡽ㏦ࡿ ࡇ ࡜ ࡟ ࡋ ࡓ ࠋ ᅗ 㸯 ࡟ &R)H ࡜ ẚ ㍑ ࡋ ࡓ,U)H ࡢ NH9 ࡢ࣐࣮࢞ࣥ⥺ࡢ␗᪉ᛶࡢ

&R ࡢⷧ࠸⟩ࢆ⏝࠸࡚ ᗘィ࡜㉸ప ᰾ᩚิࡢᗘኚ໬㸦ୖẁ㸧࡜᰾☢Ẽඹ㬆ࡢࢸࢫࢺᐇ㦂⏝ࢆවࡡࡓࡶࡢࢆ〇ࢆ♧ࡍࠋ &R)H ࡣ ᗘࡀ㸳P㹉࠶ࡓࡾࡀ୍␒ឤ

సࡋ࡚㸪◊✲࡟⏝࠸ࡿࡇ࡜࡟ࡋࡓࠋࡇࢀࡢࡁ

ᗘࡀࡼ࠸ࡀࠊ,U)H ࡣ P. ࠶ࡓࡾ࡛࠶ࡾࠊ

ᗘ࡛ᚤศࡋࡓឤᗘ ୗẁ    -55Ỉຊ↷ᑕタഛ +5     ཎᏊ᰾≀⌮Ꮫ㸪᰾≀ᛶ≀⌮Ꮫศ㔝  - 324 -

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JAEA-Review 2013-039

ࡢ 3 ྕ⅔ࢆ⏝࠸࡚⇕୰ᛶᏊࢆ↷ᑕࡋ࡚㸪㕲ࡢW(0 degree)1.0୰࡟㠀ᖖ࡟ᕼⷧ࡞ ,U)H ࢆ〇సࡋࡓࠋ ↷ᑕ
60

0.8

CoFe

ᚋࡣ 800 ᗘ࡛ࡇࡢヨᩱࢆ┿✵୰࡛ 1 ᫬㛫⇕ฎ
192

0.6

⌮ࢆࡋࡓࠋ &R&R ࡣ &R ࡢ  ࣑ࢡࣟࣥࡢ⟩ࢆ

IrFeཎ◊ࡢ 3 ྕ⅔ࢆ⏝࠸࡚⇕୰ᛶᏊࢆ↷ᑕࡋ㸪ྠᵝ࡟〇సࡋࡓࠋ

0.4

,U ࡢᙉᗘࡣ N%T ⛬ᗘ࡛㠀ᐦᑒࡢ᮲0.2

௳࡛ &(51 ࡟✵㍺ࡍࡿࡇ࡜࡟ࡋࡓࠋ᪥ᮏ࡛ࡣ /
0.0
0.001

0.01

0.1

ᆺ࡟┦ᙜࡋ࡚ࠊࡺ࠺ࣃࢵࢡ࡛㏦ࢀࡿ㔞࡛࠶ࡿࠋ
T (K)✵㍺ࡢᅜ㝿᮲⣙࡛ࡶᙉᗘࡢᙅ࠸ 5DGLRDFWLYH

dW/dT
(/K)

0DWHULDO([FHSWHG3DFNDJH81 ࡢᙇࡾ60⣬ࢆࡍࡿࡔࡅ࡛✵㍺࡛ࡁࡓࠋࡶࡕࢁࢇ &(51 ࡢ
60

40

5DGLDWLRQ6DIHW\2IILFH ࡜㸪ࡸࡾྲྀࡾࡢᚋ㸪CoFe

ཷࡅྲྀࡾチྍࢆᚓ࡚࠿ࡽ࡛࠶ࡿࠋ
㸱㸬&(51,62/'( ࡛ࡢ +I ࡢᐇ㦂20
192 IrFe &(51,62/'( ࡛ࡣ࢜ࣥࣛ࢖ࣥࡢ㉸ప ᰾ᩚ

0
0.01

0.001

0.1

ิ⿦⨨ࡀ࠶ࡾ㉁㔞ศᯒჾ࠿ࡽຍ㏿ࡉࢀࡓ +I

T (K)ࡢࣛࢪ࢜࢔࢖ࢯࢺ࣮ࣉࡀ )H ࠶ࡿ࠸ࡣ 1L ࡟ᅗ㸯.ୖẁࡣ &R)HNH9 ࣐࣮࢞ࣥ⥺࡜ẚ㍑

P. ࡢ ᗘࡢࡲࡲᡴࡕ㎸ࡴࡇ࡜ࡀฟ᮶ࡿࠋ



ࡋࡓ
ᛶࡢ



,U)H ࡢ NH9 ࡢ࣐࣮࢞ࣥ⥺ࡢ␗᪉ᗘኚ໬ࠋ ୗẁࡣࡑࢀࡒࢀ

ᗘ࡛ᚤศࡋࡓឤᗘࢆ♧ࡍࠋ
P. ࡢ㧗࡛ࡶ␗᪉ᛶࡀ࠶ࡾ㸪㧗࡛ࡶᗘィ࡜ࡋ࡚౑⏝࡛ࡁࡿࠋ 㸰㸬ヨᩱࡢ〇స,U)H ヨᩱࡣᐃྠ఩ඖ⣲ࢆཎᏊ⅔࡛↷ᑕࡍࡿࡇ࡜࡟ࡼࡾ〇సࡋࡓࠋ 㧗⣧ᗘࡢ ,U ࢆ㧗⣧ᗘࡢ㕲࡟⣙ ⁐࠿ࡋࡓࡶࡢࢆ㸦ᩘᅇ㸪㟁Ꮚࣅ࣮࣒࡟ࡼࡿ⁐⼥㸧࣮࡛ࣟࣛ⣙㸰㸮࣑ࢡᅗ㸰 10521VSHFWUXPRIP+I)Hࣟࣥⷧࡃࡋࡓࡶࡢࢆ⏝࠸ࡓࠋࡇࡢヨᩱࢆཎ◊- 325 -

3-4

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JAEA-Review 2013-039

ᐇ㦂ࡣ᭱ึࠊ༙ῶᮇ  ศࡢࢫࣆࣥ ࡢ



P

ཧ⪃ᩥ⊩

+I ࡢ࢔࢖ࢯ࣐࣮࠿ࡽጞࡵࡓࠋ P+I)H ࡢ

ࠕ㸯ࠖ60XWR72KWVXER62K\DDQG.

10521ඹ㬆ࢫ࣌ࢡࢺࣝࢆᅗ㸰࡟♧ࡍࠋ
ࡇࡢ࠶࡜
࠿ࡋ

P

+I ࡜



+I ࡢ ᐃࢆ⾜ࡗࡓࠋࡋP+I ࡣᖜᗈ࠸ࣃ࣮࣡ࣞࢰࢼࣥࢫࡢࡓࡵࠊ

1LVKLPXUD 㸪  +\S ,QWHUDFW   ࡲࡓ +I ࡣᖖ ࡛ᇙࡵ㎸ࢇࡔࡓࡵඹ㬆ࡣ ᐃ࡛ࡁ࡞࠿ࡗࡓࡀࠊ࣐࣮࢞ࣥ⥺ࡢ␗᪉ᛶ࠿ࡽ㑄ᡂᯝࡢබ⾲

⛣ࡢΰྜẚ࡞࡝ᐃ࡛ࡁࡓヲࡋ࠸ゎᯒࡣ⌧ᅾ ኱▮㐍㸪኱ᆤ㝯㸪ᖹ㔝ᬕ㄃㸪ஂಖᚭ㸪ᒣ㐍ࡵࡽࢀ࡚࠸ࡿࠋࡲࡓ௒ᖺᗘࡶᘬࡁ⥆ࡁᐇ㦂⏣ ு ኴ 㸪 Ώ 㒊 ு ኴ 㸪 す ᮧ ඞ ᙪ ,ࡀ⾜ࢃࢀ࡚ゎᯒࡀ⾜ࢃࢀ࡚࠸ࡿࠋࡇࡢᐇ㦂ࡣ

W.D.Hutchison,Ṋ⸨㇦㸸)H1Lࡢ 10521㸪ḟࡢከࡃࡢேࡓࡕ࡛⾜ࢃࢀࠊࡸࡀ࡚ṇᘧ࡞⤖᪥ᮏ≀⌮Ꮫ఍㸪➨  ᅇᖺḟ኱఍㸪 ᖺᯝࡣⓎ⾲ࡉࢀࡿணᐃ࡛ࡍࠋ &R&R ࡢ

 ᭶

ᗘィཬ

ࡧ 10521 ⏝ࡢඹ㬆ᐇ㦂ࡢሗ࿌ࡣ௒ᅇࡢሗ࿌

2.

኱▮㐍㸸ప

᰾ᩚิࢆ⏝࠸ࡓ᰾≀⌮࣭᰾࡟ࡣ㛫࡟ྜࢃ࡞࠿ࡗࡓࡀ㸪ࡇࢀ࠿ࡽ⾜࠺ணᐃ≀ᛶࡢ◊✲㸪ࠕ▷ᑑ࿨᰾࠾ࡼࡧᨺᑕ⥺ࢆ࡛࠶ࡿࠋ᭱ᚋ࡟ࡇࢀࡲ࡛ඹྠ◊✲ࢆࡸࡗ࡚ࡁ

⏝࠸ࡓ≀ᛶ◊✲㸦,㸧ࠖᑓ㛛◊✲఍㸪ி㒔ࡓከࡃࡢேࡓࡕ㸪ࡲࡓཎᏊ⅔ࡢ↷ᑕ࡟ᙜࡓࡗ

኱ᏛཎᏊ⅔ᐇ㦂ᡤ㸪 ᖺ  ᭶3-4࡚ࡣ㛤ᨺ◊ࡢⓙᵝ࡟῝ࡃឤㅰࡋࡲࡍࠋ

&(51,62/'( ࡛ࡢඹྠ◊✲⪅ྡ&6160  2UVD\ )UDQFH /5LVHJDUL&*DXODUG*$XGL
7KH8QLYHUVLW\RI2[IRUG8.1-6WRQH-56WRQH,QVWLWXW/DXH/DQJHYLQ*UHQREOH ,62/'(&(518.¸VWHU
8QLYHUVLW\RI7HQQHVVHH.QR[YLOOH86$
&%LQJKDP
8QLYHUVLW\ RI  0DU\ODQG  &ROOHJH 3DUN
86$:%:DOWHUV
1LLJDWD 8QLYHUVLW\  -DSDQ 62K\D
72KWVXER
7R\DPD8QLYHUVLW\-DSDQ.1LVKLPXUD1HXWURQ6FLHQFH/DERUDWRU\.(.7VXNXED-DSDQ60XWR
8QLYHUVLW\ RI 6XUUH\  *XLOGIRUG 8.30:DONHU$'HR=3RGRO\DN- 326 -

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JAEA-Review 2013-039

3-5తේӒ॒Ӓ୘ǛǊƣ݄ฅணƟගࡉҍൌৃƠƽǀǊȓǓȒհ࠽Ǯǽȑ݁Ҍິ༊ƣ݄Ղண‫ࢪڥ‬
Sensitive detection of alkaline cryptotephra layers in deep-sea cores from the Sea of Japan using high-resolution INAA
analysis ㇇⏛࿰ᘧ࣬௴ᚽᏰ࣬౥଱Ở ο࣬ৢறఈఉ߰࣬⠓ሪⰃႵ࣬ࠕఊॕ܎㸝໪ᾇ㐠ኬᏕ࣬ኬᏕ㝌⎌ሾ⛁Ꮥ㝌㸞.D]XKLUR7R\RGD&KXQJZDQ/LP$NDQH8PHWVX1DQDNR.DZDVKLPD<RVKLWVXJX6KLQR]XND0DVD\XNL1LWDQDL*UDGXDWHVFKRRORI(QYLURQPHQWDO6FLHQFH+RNNDLGR8QLY 㸦   ◂✪ࡡ⫴ᬊ࡛ࡐࡡណ⩇ ௙᪁ࠉ㨒㝘ᓞ୯ࡡᄂฝ㍅▴ᒒࡡ⅛⣪ᖳ௥ῼᏽ࡚ࡢࠉ ᆀ⾪ࡡᇼ✒ᒒ୯࡞ᣫࡱࡿࡒℾᒜᄂฝ∸㸝ࢷࣆࣚ㸞⌟ᅹࡻࡽ⣑஫༐ᖳ๑ࡷ⣑ඳ༐ᖳ๑࡞ࡵኬぜᶅ࡝ࣈࣝࡢࠉᗀ࠷ᆀᇡ࡚ࡡཚᐠ࡝ྜྷୌ᫤㛣㟻ࢅ♟ࡌ㘵ᒒ࡛࡝ࢼ࣭ᘟᄂℾ࠿࠵ࡖࡒࡆ࡛࠿ึ᪺ࡊ࡙࠷ࡾࠊ࡛ࡆࢀ࠿

ࡾࠊࡐࡡࡒࡴࠉ㟚㢄ࡷࢤ࢓ムᩩ࡞エ㘋ࡈࡿ࡙࠷ࡾ㧏⌿⍀‘ࡡ௙ࡡࣅࢪࢹࣤࢤ࢓࡚ࡵࡐࡡᖳ௥࡚ 7D6F Ẓᐠᗐ࡝ࢷࣆࣚᒒᗆࡡࢸ࣭ࢰࡢࠉᆀ⌣Ὼᬦ໩ࡡᑑᮮ஢

ࡡ␏ᖏࡢ᳠ฝ࡚ࡀ࡝࠾ࡖࡒࠊࡻࡖ࡙ࠉࡆࡡ㸧ࡗࡡᄂῼ࡞᭯⏕࡚࠵ࡾ࡛ࡈࡿࡾ᭩⤂ể᭿ᮆ࡝࡜ࡡẴು⃥ንℾ࡞ࡻࡾࢷࣆࣚ㜾ୖฦᕱࡢ㨒㝘㝻ᒪ㸝82NL㸞ࡡ༞けࢅᚗඔࡌࡾ୕࡚Ḗ࠾ࡎ࡝࠷ࠉ㧏ฦゆ⬗࡚㧏☔ᗐ࡝ᖳ᪁ྡྷ࡚ࡢ࡝ࡂࠉᩐ୒ᖳ๑࡞㜾ୖࡊࡒ㨒㝘ኬ࿰㸝8<P㸞

௥㍀࡛࡝ࡽ࠹ࡾࠊࡐࡡࡒࡴࠉ⫏╉࡚ࡢ᳠ฝ࡚ࡀ࡝࠷

ࢷࣆࣚࡡࡻ࠹࡞ࠉ໪け᪁ྡྷ࡞ᣉᩋ㍀ࢅࡵࡗࡡࡓࢀ࠹

࡮࡜ᕵ⷟࡝ࢷࣆࣚᒒ㸝ࢠࣛࣈࢹࢷࣆࣚ㸞ࢅࠉᆀᒒ୯

࡛᥆ῼࡊ࡙࠷ࡾࠊࡆࡿࡼࡡ⩻ᐳ࠾ࡼ᪝ᮇᾇධᇡࡡ῕

࠾ࡼຝ⋙ࡻࡂᩐኣࡂ᳠ฝࡊࠉࡐࡡࢷࣆࣚࡡ⤝″ℾᒜᾇᗇࣅࢪࢹࣤࢤ࢓ࡡᨲᑏ໩ฦᯊ࡞⮾࿝ࢅࡵࡖࡒࠊࡱ

ࢅ≁ᏽࡌࡾࡆ࡛ࠉࡱࡒྜྷୌℾᒜ࠾ࡼࡡࢷࣆࣚᒒ⩄ࢅࡒࠉ୯ᛮᏄᨲᑏ໩ἪࡢࢷࣆࣚࡡྜྷᏽἪࡡࡥ࡛ࡗ࡛ࡊ

ᄂℾẎ࡞༇ืࡌࡾᡥἪ࡞ࡗ࠷࡙ࠉけḚᕗࢅ୯ᚨ࡞┊࡙ཿࡂ࠾ࡼฺ⏕ࡈࡿ࡙࠷ࡒ࠿ࠉᮇ◂✪ࡡࡻ࠹࡞⫏╉ࢆ࡞◂✪ࡈࡿࡢࡋࡴࡒ࡛࠷࠹≟Ἓ࠿⫴ᬊ࡞࠵ࡾࠊ

࡚ࡵ☔ヾ࡚ࡀ࡝࠷⛤ࡡ⷟࠷ࢷࣆࣚᒒࡡ᳠ฝἪ࡛ࡊ࡙ ⏞ㄫ⩽ࡢ௧๑ࡡཋᏄງᶭᵋ᪃シࡡභྜྷฺ⏕ࡡᠺᯕฺ⏕ࡊࡒౚࡢࡆࡿࡱ࡚ୠ⏲࡚ࡵ᪝ᮇ࡚ࡵධࡂ࡝࠷ࡡ

࡛ࡊ࡙ᚋࡼࡿࡒࠉ⌿⍀‘ࣅࢪࢹࣤࢤ࢓ࡡ᚜㔖ඔ⣪ࡡ࡚ࠉࡐࡡ᭯⏕ᛮ࡞ࡗ࠷࡙᳠チࡊࡻ࠹࡛࠷࠹ࡡ࠿ࠉᮇ

㏻⤾ᆱ├ฦᕱࢅリࡊࡂ᳠ゞࡊࡒ࡛ࡆࢀࠉ⣑㸦୒ᖳ๑◂✪ࡡ⏞ㄫࡡ➠ୌࡡິᶭ࡚࠵ࡾࠊ

࡞㨒㝘ᓞ㸝㡉ᅗ㸞࠾ࡼᄂฝࡊࡒ㨒㝘㝻ᒪ㸝82NL㸞ࢷ ࡔ࡝ࡲ࡞ࠉ᪝ᮇาᓞ࡞㜾ୖࡌࡾ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆ

ࣆࣚᒒࡡࠉࡐࡡࡌࡃୖనࡡ  ᒒ‵࡚ࠉ82NL ࡛ྜྷᵕࣚࡡ౩⤝ℾᒜࡢࠉ᪝ᮇᾇけ❻ࡡ㡉ᅗ࣬㨒㝘ᓞ࿔㎮࡛࡝࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚࡡΊථ࡛ࡲࡼࡿࡾࢰࣤࢰࣜ㸤୯᭽ᅗሾࡡⓉ㢄ᒜࡡ㸧࢜ᡜ࡞㝀ࡼࡿࡾࠊࡆࡡ೩け㢴ࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖Ẓ㸝7D6F Ẓ㸞␏ᖏࢅ᳠ฝࡌࡾ

࡞ࡻࡖ࡙᪝ᮇ࡞ࡵࡒࡼࡈࡿࡾኬ㝛ᛮࢷࣆࣚࡢࠉ᪝ᮇ

ࡆ࡛࠿࡚ࡀࡒࠊኬ㝛ᛮࡡ࢓ࣜ࢜ࣛᒷࡢࠉ᪝ᮇาᓞࡡ

ࡡỷࡲ㎰ࡲᖈࡡᓞᘴℾᒜ࠾ࡼ౩⤝ࡈࡿࡾࢷࣆ࡛ࣚࡢ

ࡻ࠹࡝ᓞᘴℾᒜᒷ࡞Ẓ࡬࡙ࢰࣤࢰࣜྱ᭯㔖࠿ୌ᰾ኬኬࡀࡂ␏࡝ࡾ⤄ᠺࢅᣚࡗࡒࡴࠉࡐࡡ≁␏ᛮ࠾ࡼ᪝ᮇ

ࡀࡂࠉࡱࡒࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖ࡢୌ᰾࡮࡜ᑚࡈ࠷ࡆ

ࡡࢷࣆࣚ⩄ࡡ୯࠾ࡼࡡึืࡢᐖ᪾࡚࠵ࡾࠊࡐࡿ࡚ࡵࠉ

࡛࠿ኣ࠷ࡡ࡚ࠉ⢥ᗐⰃࡂ᚜㔖ඔ⣪ฦᯊࢅ㏻⤾Ⓩ࡞࠽➠ᄿ⣎ᚃ᭿࡞㨒㝘ᓞࡵⓉ㢄ᒜࡵࡐࡿࡑࡿᩐᅂ௧୕ᄂ

ࡆ࡝࠹࡛ࠉࢂࡍ࠾࡝㔖ࡡ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚࡡΊථ

ℾࡊ࡙࠷ࡾࡡ࡞ࠉᗀᇡࢷࣆ࡛ࣚࡊ࡙☔ᏽࡊ࡙࠷ࡒࡡ

࠿᳠ฝ࡚ࡀࡾ゛⟤࡞࡝ࡾࠊࡊ࠾ࡊࡆࡿࡼࡡᖳ௥࡚ࡡ

ࡢࠉ㨒㝘ᓞ࠾ࡼ⣑㸦୒ᖳ࡞㣍ᮮࡊࡒ 82NL 㨒㝘㝻㨒㝘ᓞ࡚ࡡᄂฝ㍅▴ᒒ‵ࡢ࡮࡛ࢆ࡜ሒ࿈ࡈࡿ࡙࡝࠷ࠊᒪ ࢷࣆ࡛ࣚࠉ⣑༐ᖳ๑ࡡⓉ㢄ᒜࡡኬᄂℾ࡞⏜ᮮࡌࡾ    Ț⥲ࢪ࣋ࢠࢹ࣒ࣞࢹ࣭ࣛࠉ-557 ࣂ࢕ࣈ  ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆ࡛ࣚᾇᗇᇼ✒∸ࡡᨲᑏ໩ฦᯊ                          
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㻤㻠

JAEA-Review 2013-039%7P Ⓣ㢄ᒜⱚᑚ∶ ࢷࣆࣚࡡ㸧ࡗࡡࡲ࡚ࠉ8<P ࡷ ձ ࣁࣜࢠムᩩࡡ᚜㔖ඔ⣪ฦᯊ㸯୯ᛮᏄᨲᑏ໩ฦ

%- ࡝࡜ࡡࢷࣆࣚ࡞㛭ࡊ࡙ࡢࡐࡡᄂฝᖳ௥࡞ࡢᮅࡓ

ᯊࡡ㛏ᑋ࿤ᰶ⛸ࡡῼᏽࡡࡒࡴ࡞ࠉஜ⇩⢂ᮆ࡞ࡊࡒᇼ

୘☔ᏽࡈ࠿ṟࡖ࡙࠷ࡒࠊ

✒∸ 㹢㹜ࢅ࢙࣎ࣛࢲ࡚ࣝࣤ㸨㔔࡞ᑌථࡊࡒ↯ᑏ ࡈࡼ࡞ࠉ᪝ᮇᾇ࡞࠽ࡄࡾ➠ᄿ⣎ᇼ✒∸୯ࡢ᪺ᬧⰅ

ムᩩࢅࠉ-5 ࡛ -%D ࡝࡜ࡡᵾ‵ᒷ▴ムᩩ࡛ୌ⥬࡞பᒒ࠿࠵ࡽࠉࡐࡡን㐼ࡢể᭿࡛㛣ể᭿࡚ࡡୠ⏲Ⓩ࡝

᪝ᮇཋᏄງᶭᵋ᮶ᾇ◂හࡡኬᏕ㛜ᨲ◂࡞㒉㏞ࡊ࡙ࠉᾇỀ‵ንິࡷࡻࡽ▯᭿ࡡᩐ༐ᖳ࿔᭿ࡡୠ⏲Ⓩ࡝Ẵು᮶ᾇ◂හࡡ◂✪⅌㸿㹇㹇 ࡡ 7$ Ꮗ࡚  ฦ㛣↯ᑏࢅንິ࡝࡜࡛ࡵᑊẒࡈࡿ࡙࠷ࡾࡡ࡚ࠉᆀ⌣⎌ሾን໩ࡡ౪㢏ࡊࡒࠊ↯ᑏᚃ㸦ࣦ᭮࡮࡜෫༴ࡊ࡙࠾ࡼࠉኬᏕ㛜◂✪ᑊ㇗࡛ࡊ࡙ඁⰃ࡚࠵ࡾࠊࡊ࠾ࡊࡐࡡⰅㄢࡡን໩

ᨲ◂ࡻࡽ໪ኬ࡫ᦑ㏞ࡊ࡙࠷ࡒࡓࡀࠉ໪ᾇ㐠ኬᏕኬᏕ࡞இࡊ࠷ࢤ࢓ࡵ࠵ࡽࠉ⫏╉࡚ず࠻ࡾ࢓ࣜ࢜ࣛᒷ㈹ࢷ

㝌⎌ሾ⛁Ꮥ㝌හࡡᆀୖ⟮⌦༇ᇡහࡡȚ⥲༖ᑙమ᳠ฝ

ࣆࣚᒒࡵ㝀ࡼࡿ࡙࠷ࡾࡒࡴࠉࡐࡡᒒᗆ࡞ࡢ୘᪺࡝Ⅴჹ࡚㸦ムᩩ࡞ࡗࡀஐ༐⛂㛣ῼᏽࡊࡒࠊ㸦᪝࡞⣑㸬ム࠿ṟࡈࡿ࡙࠷ࡾࠊࡐࡆ࡚ࠉ௑ᅂࠔ᪝ᮇᾇ῕ᾇᗇࢤ࢓

ᩩࡡ࣭࣋ࢪ࡚ῼᏽࢅࡊ࡙ࠉ᭿㛣හ࡚⣑ᄿ༐಴ࡡࣁࣜ

ࡡ㧏ᐠᗐ࡝ᨲᑏ໩ฦᯊ࡞ࡻࡾ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚ㜾ࢠムᩩࡡ᚜㔖ඔ⣪ฦᯊࢅ⾔ࡖࡒࠊᏽ㔖ࡊࡒඔ⣪ࡢࢠୖᒓṌࡡ㧏វᗐ᳠ฝࠕ࡛࠷࠹ᮇ㢗┘࡚ࠉཋᏄງᶭᵋ

࣑ࣞࠉࢤࣁࣜࢹࠉࢬ࣑ࣛࢗࠉࢰࣤࢰࣜࠉࢪ࢜ࣤࢩࢗ

᪃シฺ⏕භྜྷ◂✪ࡡᮇ⏞ㄫࢅ࠽ࡆ࡝ࡖࡒࠊ

࣑ࠉࣀࣆࢼ࣑ࢗࠉࣗࢗࣞࣅ࣑ࢗ࡝࡜ࡡ⣑༎ඔ⣪࡚࠵ࡾࠊ㸧 㸣◂✪ࡡ┘Ⓩ

 ղ᢫ฝࡊࡒࢷࣆࣚ⢇Ꮔࡡᨲᑏ໩ฦᯊ㸯⫏╉࡚ึ㸝㸦㸞᳠ฝࡡ᪁Ἢ ㄵࡡ᳠チ㸯ࡱࡍࠉ୯ᛮᏄᨲᑏ໩

ࡾࢷࣆࣚᒒ࡛ࠉᕵ⷟࡝ࢷࣆࣚࡡΊථࢅ♟ြࡌࡾ᚜㔖ฦᯊࢅ⏕࠷ࡒ᪝ᮇᾇᇼ✒∸୯ࡡ᚜㔖ඔ⣪ࡡ㏻⤾ᆱ├ඔ⣪⤄ᠺࡡ␏ᖏࢅ♟ࡌᇼ✒∸ムᩩ࠾ࡼࡢࠉࡨࡾ࠷࡛

ฦᕱࡡῼᏽ࠿ࠉ࢓ࣜ࢜ࣛᒷ㈹ࢠࣛࣈࢹࢷࣆࣚࡡ᳠ฝ

㔔ᾦฦ㞫ࢅ⏕࠷࡙ࠉℾᒜ࢝ࣚࢪ⢇ࡱࡒࡢ㛏▴⢇ࡡ᢫࡞≁࡞㧏វᗐ࡚࠵ࡽࠉ࠾ࡗຝ⋙Ⓩ࡚ࠉ᭯⏕࡝ᡥἪ࡚ฝࢅ࠽ࡆ࡝࠷ࠉ໪ᾇ㐠ኬᏕኬᏕ㝌⌦Ꮥ◂✪㝌හࡡ ;࠵ࡾ஥ࢅ♟ࡌࠊ

⥲ฦᯊ◂✪ᐄ࡞シ⨠ࡈࡿࡒ࢙ࢾ࣭ࣜ࢟ฦᩋᆵ (30$㸝㸧㸞ࢠࣛࣈࢹࢷࣆࣚᒒࡡ᳠ฝ㸯ḗ࡞ࠉ᪝ᮇᾇ༞

ࢅ⏕࠷࡙ࠉࡆࡿࡼࡡ⢇Ꮔࡡ୹ᠺฦฦᯊࢅ࠽ࡆ࡝ࡖࡒࠊ

㒂࠾ࡼ᪝ᮇᾇ᮶໪㒂࡞࠾ࡄ࡙ࡡ々ᩐࡡࢤ࢓ࢅ⏕࠷࡙ࠉ᚜㔖ඔ⣪ฦᯊ࡞ࡗ࠷࡙ࡢࠉ᢫ฝᠺฦ࠾ࡼࣀࣤࢺࣅࢴ

㨒㝘ᓞ࿔㎮࠾ࡼ㐛ཡ㸮୒ᖳ㛣࡞ࠉࡱࡒⓉ㢄ᒜ࠾ࡼ㐛ࢠ࡚㞗ࡴࡒࢷࣆࣚ⢇Ꮔ⣑㸦PJ ࢅ㧏⣟ᗐ▴ⱝ⟮୯࡞ཡ༎ᩐᖳ㛣࡞ࠉ᪝ᮇ࿔㎮࡞ࡵࡒࡼࡈࡿࡒ࢓ࣜ࢜ࣛᒷ

΅ᅸᑌථࡊࡒ↯ᑏムᩩࢅᵾ‵ムᩩ࡛භ࡞ࠉࣁࣜࢠム㈹ࢷࣆࣚᒒࢅࡌ࡬࡙㉦ᰕࡊ࡙ࠉ᳠ฝࡌࡾࠊ

ᩩ࡛ྜྷᵕ࡞㸿㹇㹇 ࡡ 7$ Ꮗ࡚㸫᫤㛣↯ᑏࡊࡒࠊ㸦㸝㸨㸞᳠ฝᒒࡡྜྷᏽ࡛ࢷࣆࣚ ᒒᗆࡡᵋ⠇㸯ࡈࡼ࡞ࠉ㐄㛣෫༴ᚃ࡞ᮇཋᏄງᶭᵋ᪃シහࡡኬᏕ㛜ᨲ◂ࡡȚ᳠ฝࡊࡒࢷࣆࣚᒒහ࠾ࡼ᢫ฝࡊࡒℾᒜ࢝ࣚࢪࡡฦᯊ

⥲༖ᑙమ᳠ฝჹ࡞࡙୯ᑋ࿤ᰶ⛸ࡡῼᏽࢅ࠽ࡆ࡝࠷ࠉ

࠾ࡼࠉ౩⤝ℾᒜ࡛ᄂℾẎ࡚ࡡ໩Ꮥ⤄ᠺࡡ┞㐢ࢅずࡗ㸦ࣧ᭮෫༴ᚃ࡞໪ኬ࡞㒉㏞ࡊ࡙࠷ࡒࡓ࠷࡙ࠉࣁࣜࢠ

ࡄฝࡊࡒ୕࡚ࠉᑊẒࢅ࠽ࡆ࡝࠷ࠉ᪺ᬧⰅபᒒࡡᖳ௥

ムᩩ࡛ྜྷᵕ࡞㛏ᑋ࿤ᰶ⛸ࡡῼᏽࢅ⾔ࡖࡒࠊࢷࣆࣚ⢇࡛ࡵẒ㍉ࡊ࡙ࠉࡆࡿࡱ࡚࡮࡛ࢆ࡜୘᪺࡚࠵ࡖࡒ➠ᄿᏄ୯ࡡ᚜㔖ඔ⣪ྱ᭯㔖ࡡᏽ㔖ࡢゆᯊ࠿ಞ஡ࡊ࡙ࠉゆ⣎ᚃ᭿࡞࠽ࡄࡾ᪝ᮇᾇᾇᇡ࡚ࡡ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚ

ᯊ࡞ཱིࡽ࠾࠾ࡖ࡙࠷ࡾࠊ

ᒒᗆࢅ☔❟ࡌࡾ஥ࢅ┘Ⓩ࡛ࡊࡒࠊ 㸝㸧㸞ฦᯊムᩩ㸨㸣◂✪ࡡ᪁Ἢ ձ ฦᯊ࡞⏕࠷ࡒムᩩࡢ୹࡛ࡊ࡙᪝ᮇาᓞἚ࠷ࡡ

㸝㸦㸞ฦᯊᡥἪ

᪝ᮇᾇ࡞࠽ࡄࡾ⏐ᴏᢇ⾙⥪ྙ◂✪ᡜᡜ᭯ࡡࣅࢪࢹࣤ

3-5


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㻤㻡

JAEA-Review 2013-039

ࢤ࢓࡚࠵ࡾࠊ┘Ⓩ 㸦 ࡞ࡗ࠷࡙ࡢࠉ௧ୖࡡ㸪ࡗࡡࢤ

82NL ࢷࣆࣚᒒᗆ࡚࠵ࡾࠊ

࢓୯ࡡ࠷ࡍࡿࡵ㐛ཡᩐ༐ᖳࠤ⣑㸧୒ᖳ๑ࡡᇼ✒ᖳ௥࡞┞ᙔࡌࡾ㒂న࠾ࡼ㏻⤾ࡊ࡙㸦FP 㛣㝰࡚᤿ཱིࡊࡒ
⣑༐஦Ⓤ಴ࡡムᩩ࡞ࡗ࠷࡙᚜㔖ඔ⣪ฦᯊࢅ⾔ࡖࡒࠊ ࣬*+'㸯ᓞ᰷ἀ ᑊ㤷ᾇ⓽༞㒂 ࢤ࢓ FP
࣬*+3㸯  㝻ᒪ໪᮶᪁ ኬ࿰ᾇ⓽༞け❻ ࢤ࢓ FP
࣬*+㸯㫵ཱིἀࢤ࢓ FP
࣬*+.7୸ᚃ༖ᓞἀࢤ࢓FP
࣬*+㸯㔘Ἁἀ ໪㝛ἀ⦍㎮ྋᆀ ࢤ࢓ FP ղ ḗ࡞ࠉ┘Ⓩ㸝㸧㸞࡛㸝㸨㸞࡞ࡗ࠷࡙ࡢࠉ᪝ᮇᾇỞ ᅒ᪝ᮇᾇ༞ᾇᇡࡡ㸪ࢤ࢓୯ࡡ 7D6F ᆱ├ฦᕱ༞᮶㒂ࡡ໪㝛ἀࠉኬ࿰ᾇ⓽ࠉᒜ㝔ἀࡡ㸪ࡗࡡࢤ࢓୯

࠾ࡼࠉ㐛ཡ㸧ࠤ㸮୒ᖳ๑ཧࡢ⣑㸬୒ᖳࡱ࡚ࡡᖳ௥ࡡ ୌ␊けࡡᾇᇡ࡚᤿ཱིࡈࡿࡒ㸝ᅒ㸦ࡡᕞ❻ࡡ㸞ࢤ࢓㒂న࠾ࡼ㏻⤾ࡊ࡙㸦FP 㛣㝰࡚ฦཱིࡊࡒ⣑༐஫Ⓤムࢅ㝎ࡂ㸩ࡗࡡࢤ࢓࡞ࡗ࠷࡙ࠉ82NL ᒒ௧አ࡞ࡵࢰࣤ

ᩩ࡞ࡗ࠷࡙᚜㔖ඔ⣪ฦᯊࢅ࠽ࡆ࡝࠷ࠉ㨒㝘ᓞ࿔㎮࠽ࢰࣜࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖Ẓ࠾ࡼࡐࡿࡑࡿ㸦ࠤ㸨ᒒࡻࡦⓉ㢄ᒜࢅ౩⤝ℾᒜ࡛ࡊࡒ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚࡡ

ࡡ ໩ Ꮥ Ⓩ࡝ ␏ ᖏ ᒒ ࠿ ᳠ ฝ ࡈ ࡿࡒ ࠊ ࡆ ࡿ ࡼ ࡢ ࣈࣝ᳠ฝࢅ⾔ࡖࡒࠊ

82NL ࡷ࣎ࢪࢹ 82NL ࡛ࡆࡿࡱ࡚࿣ࡣࡿ࡙࠷ࡒࠉࡐ ࣬*+1ᒜ㝔ἀࢤ࢓ FP

ࡡᏋᅹ࠿୘☔࠾࡝࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚ࡞┞ᙔࡌࡾྊ ࣬*+໪㝛ἀ㸝ኬ࿰ᾇ⓽㸞FP⬗ᛮ࠿㧏࠷ࠊࡐࡡ␏ᖏᒒ࠾ࡼ᢫ฝࡊࡒ⢊⢇࡝⢇Ꮔ࡞ ࣬*+໪㝛ἀ㸝ኬ࿰ᾇ⓽㸞FPࡗ࠷࡙㢟᚜㙶びᐳ࡛ (30$('6 ฦᯊࢅ࠽ࡆ࡝ࡖࡒ⤎ ࣬*+㸯⏠㮭༖ᓞἀ㸝ኬ࿰ᾇ⓽㸞FP

ᯕࠉࡐࡡ⢊⢇⢇Ꮔ୯ࡡ 㸚࠿㨒㝘ᓞ⣌ℾᒜࢅ⤝″࡛ ࣬*+ ⏠㮭༖ᓞἀ ఫῳᾇᕃ㎾എ FP

ࡌࡾ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚ⢇࡛ึᏽࡈࡿࡒࠊࡗࡱࡽ⫏ ճ ࡈࡼ࡞ࠉ㐛ཡ༎ᩐ୒ᖳ㛣ࡡ᭽㩥༖ᓞ໪㒂Ⓣ㢄ᒜ╉࡚ࡢ≁ᏽ࡚ࡀ࡝࠷࡮࡜ᕵ⷟࡝࢓ࣜ࢜ࣛᒷ㈹࣏࢕ࢠ

ࢅ౩⤝″࡛ࡌࡾ࢓ࣜ࢜ࣛᒷ㈹ࡡᗀᇡࢷࣆࣚࡡ᳠ฝࢅ

ࣞࢷࣆࣚᒒ࠿᚜㔖ฦᯊ࠾ࡼ᳠ฝ࡚ࡀࡾᐁౚࢅᣪࡅࡾ

⾔࠹ࡒࡴࠉ㏻⤾ࡊ࡙㸦FP 㛣㝰࡚ฦཱིࡊࡒ༐ᩐⓊムᩩ஥࠿࡚ࡀࡒࠊ

࡞ࡗ࠷࡙ࡡ᚜㔖ඔ⣪ฦᯊ࠿࡮࡯⤂ࢂࡖࡒṹ㝭࡚࠵ࡾࠊ ࡈࡼ࡞ࠉ⣑୏༐୔Ⓤᖳ๑࡞け᪝ᮇ࡞ᗀࡂ㜾ୖࡊࡒ

࣬.53& ᮿ๑ᾇྋFP㨛⏲࢓࢜࣌ࣕ㸝.$K㸞ࡡࢷࣆࣚᒒ࠿☔ヾ࡚ࡀࡒࡡࡢࠉ

࣬.53& ⏻ⴄἀ ᪝ᮇᾇ⓽ ゆᯊ୯㸪ࡗࡡࢤ࢓ࡡ࠹ࡔࡡୌࡗ㸝ᅒ㸧ࡡ୯ኳ㸞ࡓࡄ࡚࠵ࡾࠊ

࣬*+ ⩒ᖙἀ ᪝ᮇᾇ⓽ FP

.$K ࢷࣆࣚࡢ᪝ᮇᾇᇼ✒∸࡞Ẓ࡬࡙ࢠ࣑ࣞྱ᭯㔖࠿ᑚࡈ࠷ࡡ࠿ࡐࡡ໩Ꮥ⤄ᠺࡡ≁ᚡ࡚࠵ࡾࠊࡐࡡࢤ࢓

㸩㸣◂✪ᠺᯕ

௧አࡡ㸨ࡗࡡࢤ࢓୯ࡡࢠ࣑ࣞࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖㸝㸦㸞ࢠࣛࣈࢹࢷࣆࣚ᳠ฝࡡ᭯ຝᛮࡡ᳠チẒࡡᆱ├ฦᕱ㸝ᅒ㸧㸞࡞ࡢࠉ.$K ࢷࣆࣚࡡΊථࢅ♟ ᪝ᮇᾇ༞㒂ࡡ㸪ᮇࡡᾇᗇࢤ࢓୯ࡡᩐ༐୒ᖳ࠾ࡼ㸦ြࡌࡾ໩ᏕⓏ␏ᖏᒒ㸝ᅒ㸧୯ࡡ▦༰ $%& ࡐࡊ࡙ '㸞୒ᩐ༐ᖳ๑ࡡᇼ✒ᒒࡡࣁࣜࢠฦᯊࡡࢰࣤࢰࣜࢪ࢜

࠿᳠ฝࡈࡿࡒࠊࡆࡿࡼࡡࢠ࣑ࣞࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖ࣤࢩ࣑ࢗྱ᭯㔖Ẓࡡᆱ├ฦᕱࢅᅒ㸦࡞♟ࡌࠊ࡝࠽ࠉ

Ẓࡡ␏ᖏᒒ࠾ࡼ᢫ฝࡈࡿࡒ⢊⢇ࡡὮ⣘ᒷ㈹ℾᒜ࢝ࣚᅒ 㸦 ୯ ࡡࣀ ࢴ ࢲ ࢅ ࠾ ࡄ ࡒ ᒒ ࠿⫏ ╉ ࡚ ☔ ヾ ࡈ ࡿࡒࢪ⢇࡛㛏▴࡞ࡗ࠷࡙ࠉᑿᢙ⋙ῼᏽ㸝௺ᴏ࡞ῼᏽ౪㢏㸞3-5


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࡛ (30$('6 ฦᯊ㸝ᅒ㸨㸞ࢅ⾔ࡖࡒ⤎ᯕࠉࡐࡡ 㸚 ࡈࡼ࡞ࠉ᪝ᮇᾇけ༞㒂࡞࠽ࡄࡾ㐛ཡ㸧୒ᖳ㛣ࡡ࢓ࡡ⢇Ꮔ࠿ .$K ࡛࠷࠹ࢷࣆࣚᠺฦ࡛≁ᏽࡈࡿࡒࠊ

ࣜ࢜ࣛᒷ㈹ࢷࣆࣚᒒᗆࢅ☔ᏽࡌࡾࡒࡴ࡞ࡢࠉ᢫ฝࡊ
ࡒࢷࣆࣚ⢇ࡡᄂℾẎ࡚ࡡ᚜㔖ඔ⣪ࣂࢰ࣭ࣤࡡ┞㐢ࢅず࠷ࡓࡌࡆ࡛ࡵᚪこ࡚ࠉ⌟ᅹゆᯊ୯࡚࠵ࡾࠊ 㸝 㸧 㸞 ᪝ ᮇᾇ ༞ ᮶㒂 ࡚ ࡡ 㐛ཡ 㸮 ୒ᖳ 㛣 ࡡ ࢓ࣜ ࢜
ࣛᒷ㈹ࢷࣆࣚᒒᗆࡡᵋ⠇ ḗ࡞ᮇᡥἪࢅ⏕࠷࡙ࠉᒜ㝔ἀࢤ࢓㸦ᮇ࡛᮶໪ᆀ᪁けᓃࢤ࢓㸩ᮇ࡞࠽ࡄࡾ㸨ࠤ㸮୒ᖳ๑ࡡᖳ௥࡚ࡡᒒࢅ
㉦ᰕࡊࡒ࡛ࡆࢀࠉࢰࣤࢰࣜࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖Ẓࡡᆱ├ฦᕱ㸝ᅒ 㸞࡞࠵ࡾࡻ࠹࡞ࠉ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆ

ᅒ㸧᪝ᮇᾇ༞ᾇᇡࡡ㸪ࢤ࢓୯ࡡ &U6F ᆱ├ฦᕱࣚࡡΊථࢅ♟ࡌኣᩐࡡ໩ᏕⓏ␏ᖏᒒ࠿᳠ฝࡈࡿࡒࠊ
ࡐࡡ␏ᖏᒒࡡ࡮࡛ࢆ࡜ࡢ⫏╉࡚ࡢ☔ヾ࡚ࡀ࡝࠷ࡵࡡ
࡚࠵ࡽࠉࡱࡒࡵ࠹ࡥ࡛ࡗࡡᖳ௥ỬᏽἪ࡛ࡊ࡙ࡻࡂ౐
⏕ࡈࡿࡾ᪺ᬧⰅபᒒࡵࡷࡷ୘᪺▉࡝ࡒࡴࠉ᪺ᬧⰅப
ᒒᒒᗆࡡࡲ࡚☔ᐁ࡝ᖳ௥☔ᏽࢅࡌࡾࡡࡢ㞬ࡊ࠷ࢤ࢓࡚࠵ࡾࠊᅒ㸩 ᪝ᮇᾇ᮶༞ᇡࡡ㸪ࢤ࢓୯ࡡ 7D6F ᆱ├ฦᕱᅒ㸨᢫ฝ㖌∸ࡡ୹ᠺฦ⤄ᠺ D ℾᒜ࢝ࣚࢪ㸝E㸞㛏▴ ᮇᡥἪ࡞ࡻࡖ࡙᳠ฝࡈࡿࡒࢠࣛࣈࢹࢷࣆࣚᒒ࡛⫏╉࡚☔ヾ࡚ࡀࡾࢷࣆࣚᒒ࡛ࡡ┞㐢ࡢࠉࢷࣆࣚᠺฦࡡ
௙ࡡᇼ✒∸ᠺฦ࡞ࡻࡾᕵ㔐⋙ࡓࡄ࡚࡝ࡂࠉࢷࣆࣚ⢇Ꮔࡡ⢇ᗐࡡ㐢࠷࡞ࡻࡽ⏍ࡋࡾ࡛⩻࠻ࡼࡿࡾࠊᮇムᩩ୯ࡡ⫏╉࡚☔ヾ࡚ࡀࡾࢷࣆࣚᒒ୯ࡡࢷࣆࣚ⢇Ꮔࡢ
PP ࡻࡽࡵ⢊⢇࡚࠵ࡾࡡ࡞ᑊࡊ࡙ࠉᮇᡥἪ࡚᳠ฝ
ࡈࡿࡒࢠࣛࣈࢹࢷࣆࣚᒒ୯ࡡࢷࣆࣚ⢇ࡡኬ㒂ฦࡢPP ௧ୖࡡኬࡀࡈ࡚ࠉࡐࡡ᢫ฝ࡛ฦ㞫࡞ࡢ㸦ムᩩ࡚ࡵ┞ᙔ࡝᫤㛣࡛ᡥ㛣࠿ᚪこ࡛࡝ࡾࠊᮇἪࡢࢷࣆ
ࣚᠺฦ࡛ࡐࡿ௧አࡡᇼ✒∸ᠺฦ࡛ࡡ㛣ࡡኬࡀ࡝໩Ꮥ
⤄ᠺࡡ┞㐢ࢅฺ⏕ࡊ࡙ࠉ᪝ᮇᾇᇼ✒∸୯ࡡ㔔㔖Ẓ࡚ ࡆࡿࡼࡡ␏ᖏᒒࡡ⢊⢇┞࠾ࡼฦ㞫ࡊࡒℾᒜ࢝ࣚࢪ୯ࡡ୹ᠺฦඔ⣪ࡡᏽ㔖㸝ᅒ 㸞ࢅ⾔࠹ࡆ࡛࡚ࠉࡐࡡ
ࢠࣛࣈࢹࢷࣆࣚ࠿ࠉ㨒㝘ᓞ⣌ࢷࣆࣚ࠾Ⓣ㢄ᒜ⣌ࢷࣆࣚ࠾ࠉࡱࡒࡢࢰࣤࢰࣜࢪ࢜ࣤࢩ࣑ࢗྱ᭯㔖Ẓ࠿ࡷࡷ㧏࠷ࡡ࠿≁ᚡ࡚࠵ࡾ $VR 㜷⸵㸩 ࢷࣆࣚ࡝ࡡ࠾ࢅ
༇ืࡌࡾ஥࠿࡚ࡀࡾࠊ

⣑㸧㸚࡞ᕵ㔐ࡈࡿࡒ㨒㝘ᓞ⣌ࢷࣆࣚᒒ࡚ࡵ᳠ฝ࡚ࡀ

3-5

ࡾ஥ࢅᐁチ࡚ࡀࡒࠊ

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௥ࡢࠉ8<P࠿  ༐ᖳ๑ࠉ%- ࠿  ༐ᖳ๑ࠉ
༐ᖳ๑ࠉ ༐ᖳ๑ࠉ ༐ᖳ๑࡛゛⟤ࡈࡿࡒ㸝ᅒ㸞ࠊ᢫ฝࡊࡒࢷࣆࣚ⢇୯ࡡ᚜㔖ඔ⣪ࡡᏽ㔖ࡵ࡮࡯⤂ࢂࡖ࡙࠽ࡽࠉ⌟ᅹࠉ⤝″ℾᒜࡡ㐢࠷ࡓࡄ࡚࡝ࡂࠉࡐ
ࡿࡑࡿࡡ⤝″ℾᒜࡡᄂℾẎ࡚ࡡ᚜㔖ඔ⣪ࣂࢰ࣭ࣤࡡ
┞㐢࡞ࡗ࠷࡙ゆᯊ୯࡚࠵ࡽࠉࡆࡿࡼࡡ⤎ㄵ࡞ࡗ࠷࡙
ࡵᅗ㝷Ꮥ⾙㞟ヽ࡞ᢖ✇‵ങ୯࡚࠵ࡾࠊ㸝 㸨 㸞 ᪝ ᮇᾇ ໪ ᮶㒂 ࡚ ࡡ 㐛ཡ 㸦 㸪୒ ᖳ 㛣 ࡡⓉ 㢄ᒜ⣌ࢷࣆࣚᒒᗆࡡᵋ⠇ᅒ㸪᢫ฝࡊࡒℾᒜ࢝ࣚࢪࡡ୹ᠺฦ⤄ᠺ࡛౩⤝ℾᒜ ࡈࡼ࡞ᮇἪࢅ⏕࠷࡙ࠉ໪ᾇ㐠けᓃࡡ㸧ࡗࡡ᪝ᮇᾇ
ࢤ࢓හࡡ ࠤ ୒ᖳ๑ࡡᒒ࡞ࡗ࠷࡙ྜྷᵕ࡞㉦ᰕࡊࡒ ᒒᗆᏕⓏ࡝⩻ᐳ࠾ࡼࠉ8<P㸝㨒㝘ኬ࿰㸞ࢷࣆࣚࢅྱࡳ࡚࠵ࢀ࠹㸧ᒒࡡ㨒㝘ᓞ⣌ࢷࣆࣚࠉ࠽ࡻࡦ %-㸝Ⓣ㢄ᒜ᪝ᮇᾇ⓽㸞ࢷࣆࣚࢅྱࡳ࡚࠵ࢀ࠹㸨ᒒࡡⓉ㢄ᒜ⣌ࢷࣆࣚᒒ࠿ࠉࡐࡿࡑࡿ㸨ࡗࡡࢤ࢓࠾ࡼ᳠ฝࡈࡿࡒ
࡛⩻࠻ࡼࡿࡾࠊ᩺ࡊࡂ᳠ฝ࡚ࡀࡒࢷࣆࣚࡢ 8$NL 㨒㝘⚽⏛ἀ ࠉ%$NL 㨒㝘⚽⏛ἀ ࠉ%V$VR $VR࡛ࡆࢀࠉ ༐ᖳ๑ࡡ %9㸝Ⓣ㢄ᒜࢗࣚࢩ࢛ࢪࢹࢴࢠ㸞ࠉ%- ࠽ࡻࡦ๑㏑ࡡ %Ѹ$NL ࡛ %V$VR ࡡࢷࣆࣚࢅྱࡳ ᒒࡡ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚᒒ࠿᳠ฝࡈࡿ࡙࠽ࡽࠉࡆࡿ
ࡼࡢ୹ᠺฦඔ⣪ฦᯊࡡ⤎ᯕࠉࡌ࡬࡙Ⓣ㢄ᒜ⣌ࢷࣆࣚᒒ࡛ึ᪺ࡊࡒࠊࡆࡆ࡚᩺ࡒ࡞᳠ฝࡈࡿࡒ㸧ࡗࡡⓉ㢄ᒜ⣌ࢷࣆࣚࡡᖳ௥ࡢࠉࡆࡡࢤ࢓ࡡ᪺ᬧⰅபᒒᒒᗆ㸝ờ
ཋࠉᮅⓆ⾪ࢸ࣭ࢰ㸞࠾ࡼ⿭㛣ࡊ࡙  ༐ᖳ๑࡛ ├ᚃࡡ㨒㝘⣌ ࡛ࡐࡿࡑࡿ࿤ྞࡊࡒࠊ༐ᖳ๑࡛゛⟤ࡈࡿࡾࠊࡆࡿࡼࡡᒒ࠾ࡼ᢫ฝࡊࡒࢷࣆ
ࣚ⢇୯ࡡ᚜㔖ඔ⣪ࡡᏽ㔖ࡌࡾࡆ࡛࡚ࠉࡈࡼ࡞Ⓣ㢄ᒜࡡリࡊ࠷ᄂℾᒓṌࡷ࣏ࢡ࣏‸ࡱࡽࡡ໩Ꮥ⤄ᠺࡡን໩ࢅ්⌟࡚ࡀࡾྊ⬗ᛮࢅ♟ြ࡚ࡀࡿࡣ࡛⩻࠻࡙࠷ࡾࠊ
㸪㸣ࡆࡿࡼࡡᠺᯕ࡞ᑊࡌࡾビ౮࡛௑ᚃࡡ᪁ 㔢 ௧୕ࡡ◂✪ᠺᯕ࡚ࡢࠉ㎾ᖳἸ┘ࡈࡿ࡙࠷ࡾࢠࣛࣈ
ࢹࢷࣆࣚࡡ㧏វᗐ࡝᩺᳠ฝἪࢅ♟ࡊࠉࡐࡿ࠿ຝ⋙Ⓩ
࡝ᡥἪ࡚࠵ࡾ஥ࢅ᪝ᮇᾇࡡᇼ✒∸࡚ᐁチࡊ࡙ࠉ᪝ᮇ
ᅒ㸫᪝ᮇᾇ᮶༞ᾇᇡࡡ㸪ࢤ࢓୯ࡡࢷࣆࣚᑊẒࡡ➠ᄿ⣎ᚃ᭿ࡡ࢓ࣜ࢜ࣛᒷ㈹ࢷࣆࣚᒒᗆࢅ☔❟ࡊࡗࡗ࠵ࡾࡆ࡛ࢅ♟ࡊࡒࠊ◂✪ᠺᯕ㸝㸦㸞ࡢ᪜࡞ ࡆࡿࡼࡡ᳠ฝᒒ࠾ࡼ᢫ฝࡊࡒࢤ࢓㛣࡚ࡡ྘ࢷࣆࣚ

*HRFKLPLFDHW&RVPRFKLPLFD$FWD ࡛࠷࠹ୌὮࡡᅗ

ᒒࡡᑊẒࢅ࠽ࡆ࡝࠹஥࡚ࠉムᩩࢤ࢓୯ࡡ୘᪺▉࡝᪺㝷Ꮥ⾙㞟ヽ࡞᥎㍍ࡈࡿ࡙࠽ࡽࠉ◂✪ᠺᯕ㸝㸧㸞࡛㸝㸨㸞ᬧⰅபᒒࡡᖳ௥ࡵୌ㒂☔ᏽࡌࡾ஥࠿࡚ࡀࡒࠊ$7㸝ጳ࡞ࡗ࠷࡙ࡵࠉ᢫ฝࡊࡒࢷࣆࣚ⢇୯ࡡ᚜㔖ඔ⣪ྱ᭯㔖Ⰳ㸞ࢷࣆࣚࢅ  ༐ᖳ๑ࠉ$VR ࢷࣆࣚࢅ  ༐ᖳࡡゆᯊ࠿Ᏸ஡ḗ➠ࠉࡐࡿࡑࡿ୹こ࡝ᅗ㝷Ꮥ⾙㞟ヽ࡞๑ࡡᄂฝࠉ7/ ᬧⰅᒒ  ࡡᗇ㟻ࡡᖳ௥ࢅ  ༐ᖳᢖ✇ࡌࡾࡻ࠹࡞‵ങ୯࡚࠵ࡾࠊ⌟ᅹ᛬ຸ࡛ࡈࡿ࡙࠷

๑࡛ࡊ࡙ᖳ௥ࢅ⿭㛣ࡌࡾ࡛ࠉࡐࡿࡑࡿࡡࢷࣆࣚࡡᖳ

ࡾ᭩⤂ể᭿ᮆࡡẴು⃥ንࡡ᪝ᮇ㎾㑱࡛ୠ⏲྘ᆀ࡛ࡡ3-5

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᫤㛣Ⓩ࡝ࡍࡿࠉཀྵࡦẴು⃥ንࡡᶭᵋࡡゆ᪺ࡷࠉ᭩⤂ể᭿ᮆࡡ᪝ᮇ࿔㎮ࡡᾇὮ࡛ᾇ㟻ࡡን໩࡞ࡗ࠷࡙ࡡ⥽ᠺ ᯕࡡප⾪㸝   㸞㸪㸣ᠺᖳࢅ࠽ࡆ࡝࠹୕࡚ࡵࠉᮇ◂✪ࡢ㔔こ࡝ᙲ๪ࢅᯕࡒࡌࠊ

ࠜ㞟ヽㄵᩝࠝ

ࡆࡡ᩺ᡥἪࢅὩ⏕ࡌࡾࡆ࡛࡚ࠉୠ⏲ࡡ௙ࡡὩິⓏ⦍

ձ/LP&,NHKDUD.7R\RGD.&U\SWRWHSKUD

㎮㒂ᆀᖈ࡞࠽ࡄࡾࢷࣆࣚᒒᗆࡵ㣍㌅Ⓩ࡞⢥ᐠ࡞࡝ࡽࠉ

GHWHFWLRQXVLQJKLJKUHVROXWLRQ㐛ཡࡡᆀ⌣⎌ሾንິࡡᚗඔ࡞ᐞ୙ࡌࡾ஥࠿᭿ᙽࡈࡿ

WUDFHHOHPHQW DQDO\VLV RI +RORFHQH PDULQHࡾࠊ

VHGLPHQWV VRXWKZHVW -DSDQ *HRFKLPLFD HW ௑ᚃࠉࡈࡼ࡞ࠉᮇᠺᯕࢅᢪࡊ㐅ࡴ࡙ࠉ㐛ཡ㸨㸥୒

&RVPRFKLPLFD$FWDᖳ㛣ࡡけ᪝ᮇ࡞࠽ࡄࡾ㧏ᐠᗐ࡝ࢷࣆࣚ࢜ࢰࣞࢡ࣬᚜

㔖ඔ⣪ࢸ࣭ࢰ࣭࣊ࢪࡡషᠺࢅ┘Ⓩ࡞ࠉᖲᠺ㸧㸦ᖳᗐ

ࠜᏕఌⓆ⾪ࠝ

࠾ࡼࠔ⌿⍀‘ᤸ๎ࢤ࢓ࡡℾᒜ⅂㜾⅂ᒒ‵୯ࡡℾᒜ࢝ձ௴ᚽᏰࠉờཋ◂ࠉ㇇⏛࿰ᘧࠉ᪝ᮇᾇᇼ✒∸ࢤ࢓ࡡࣚࢪࡡᨲᑏ໩ฦᯊࠕ࡛࠷࠹㢗┘࡚ࠉᮇཋᏄງᶭᵋ᪃

୯ᛮᏄᨲᑏ໩ฦᯊ࡞ࡻࡾ➠ᄿ⣎ᚃ᭿ࡡ࢓ࣜ࢜ࣛ

シࡡභྜྷฺ⏕ࢅ⏞ㄫࡊུ࡙⌦ࡈࡿࡒࡡ࡚ࠉ ᭮࠾ࡼ

ᒷ㈹ࢷࣆࣚᒒᗆࡡᵋ⠇ࠉ᪝ᮇᆀ⌣໩Ꮥఌ  ᖳཋᏄ⅌ࡡ㐘㌷࠿්㛜ḗ➠ࠉῼᏽࢅ㛜ጙࡊࡒ࠷ࠊ

ఌࠉ ᖳ  ᭮  ᪝ࠉ㥎ሔ㸝᮶ா㸞ᖳ࡞⌿⍀‘୯ኳ㒂࡞࡙ᤸ๎ࡈࡿࡒ P ⣥ࡡ‘ᗇᇼ

ղ&KXQJZDQ/,0ࠉ.D]XKLUR72<2'$ࠉ.HQ,.(+$5$ࠉ

✒∸ࢤ࢓ࡢࠉᮇሒ࿈᭡ࡡ᪝ᮇᾇࢤ࢓࡛ࡢ␏࡝ࡽࠉⰴ

&U\SWRWHSKUD GHWHFWLRQ E\ KLJKUHVROXWLRQ⢂ฦᯊࡷ⌓⸬ฦᯊࠉ᭯ᶭ໩Ꮥฦᯊ➴ࡡኣᩐࡡ㡧┘࡞

WUDFHHOHPHQWࡗ࠷࡙ྜྷୌࡡムᩩ࡞㛭ࡊ࡙㧏ฦゆ⬗࡞ゆᯊ࠿⾔ࢂࡿ

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LQWKH-DSDQ6HDࠉ᪝ᮇ➠ᄿ⣎Ꮥఌ  ࿔ᖳエᛍࡇᩅ♟࠷ࡒࡓ࠷ࡒࠊᚨࡻࡽ࠽♡ࢅ⏞ࡊ୕ࡅࡾࠊࡈࡼ

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- 332 -

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8OUHXQJLVODQG.RUHDࠉ᪝ᮇ➠ᄿ⣎Ꮥఌ  ࿔ᖳエᛍᅗ㝷ࢨࣤ࣎ࢩ࣑ࢗ  ᖳ  ᭮  ᪝ࠉ⏐⥪◂㸝➻ἴ㸞

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3-5- 333 -

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JAEA-Review 2013-039

3-6
ᾏỈ‽ኚືሁ✚≀ࡢ⺯ගᖺ௦ᐃ࡜ᨺᑕ໬ศᯒ࡟ࡼࡿᖺ㛫⥺㔞

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*Hakodate School, Hokkaido University of Education㸬ࡣࡌࡵ࡟

࡛ᫎࡁ࡞࠸ሗ࿌࡟࡞ࡿࡇ࡜ࢆணࡵグࡋ࡚࠾ⅆᒣ▼ⱥࡢ 5 7 / 㸦㉥⇕⺯ග㸧◊✲ࡣࡁࡓ࠸㸬+DVKLPRWRHWDO  ࡸ0LDOOLHUHWDO

ᮏㄽ࡛ࡣ0XUUD\DQG:LQWOH  ࡀᥦၐ ࡟ࡼࡗ࡚㛤ጞࡉࢀࡓ㸬57/ࡣᆅࡋࡓ༢࢔ࣜࢥࢵࢺ෌⌧ἲ 6$5 ἲ ࢆ᥇⏝ࡋࡓ㸬㉁ᖺ௦

ࡲࡓ㸪ᨵⰋࡉࢀࡓ 57/ ⿦⨨ࢆ⏝࠸୍࡚⢏Ꮚ࡟ᐃ࡟ඃࢀࡓᇶᮏⓗ࡞ᛶ㉁ࢆ᭷ࡋ࡚࠾

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ࣛࢵࣉ㟁Ꮚࡢ␗ᖖᾘኻࡢ୙Ꮡ࡞࡝࡛࠶ࡾ㸪ND໭ᾏ㐨࡟఩⨨ࡍࡿὝ√࢝ࣝࢹࣛ࠿ࡽᄇฟࡋࡓ

࠿ࡽ0D࡟ཬࡪᗈ࠸᫬௦ࡢᖺ௦ ᐃࡀྍ⬟Ὕ√ⅆ○ὶሁ✚≀࡛࠶ࡿ㸬ᐃࢆヨࡳࡓ⤖ᯝ࡟ࡘ࠸࡚ሗ࿌ࡍࡿ㸬࡜ ࡉ ࢀ ࡚ ࠸ ࡿ )DWWDKL DQG 6WRNHV 
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ຍ⇕⿦⨨࠿ࡽᨺฟࡉࢀࡿࣂࢵࢡࢢࣛ࢘ࣥࢻࢩ

᪥ᮏࡢ୺せ࡞⃭ࡋ࠸ⅆᒣάືࡢ୍ࡘ࡛㸪ᄇฟࢢࢼࣝ࡜ศ㞳ࡍࡿసᴗࡣ㸪ヨᩱ57/ᐃࡢせࢸࣇࣛ㔞ࡣ7SIOⅆ○ὶNP࡜7SID㝆ୗࢸ࡜࡞ࡗ࡚࠸ࡿ㸬ࡇࢀࢆ㐩ᡂࡍࡿࡓࡵ㸪ࣇ࢕ࣝࣇࣛNP࡛㸪ྜィNP࡟࠾ࡼࡪ㸦0DFKLGDࢱ࣮⤌ࡳྜࢃࡏ㸪㐺ษ࡞307ࡢ฼⏝㸪ࡑࡋ࡚

DQG$UDL㸧 )LJDE 㸬Ὕ√࢝ࣝࢹࣛ

57/ ᳨ฟ⿦⨨ࡢᨵၿ࡞࡝ࡢᢏ⾡ᨵⰋࡶ㐍ࡵࡽࡢ࿘㎶㸦[NPࡢ⠊ᅖ㸧ࡣ㸪࡞࠸ࡋᒙࢀ ࡚ ࠸ ࡿ +DVKLPRWR  <DZDWD DQGࡢཌ࠸ⅆ○ὶࣘࢽࢵࢺ࡟そࢃࢀ㸪ྛࣘࢽࢵࢺ+DVKLPRWR 㸬ࡣᣳᅾࡍࡿ㝆ୗࢸࣇࣛࡸࣛࢢࣈࣞࢩ࢔࡛༊ศ

ࡲࡓ㸪ᖺ㛫⥺㔞ࢆồࡵࡿࡓࡵ࡟㸪୍⯡࡟ࡣࡍࡿࡇ࡜ࡀ࡛ࡁࡿ㸬ᡃࠎࡢ㔝እㄪᰝ࡛ࡣ㸪Ὕ,&3 ࣐ࢫ➼ࡢ᪉ἲࡀྲྀࡽࢀࡿࡀ㸪ᡃࠎࡣ 8 ࠾√࢝ࣝࢹࣛࡢ༡ഃ㸪ⅆ○ὶሁ✚≀ᒙᗎࡢࢱ࢖

ࡼࡧ 7K ࡢṇ☜࡞ ᐃࢆ⾜࠺ࡓࡵ࡟㸪ཎᏊຊᶵ

ࣉᆅⅬ㸪㛗ὶᕝὶᇦ࡟࠾࠸࡚㸪7SIOࡣ㐃⥆ᵓ᪋タࡢ -55 ࢆ฼⏝ࡋࡓ୰ᛶᏊᨺᑕ໬ศᯒ

ⓗ࡞ࣘࢽࢵࢺ࠿ࡽ࡞ࡾ㸪ୗ఩ࡼࡾ7SIO$ࢆ㐍ࡵ࡚࠸ࡿ㸬ࡋ࠿ࡋ㸪ṧᛕ࡞ࡀࡽ㸪᪋タᨾ

7SIO%࡜7SIO&࡟༊ศࡉࢀࡿ )LJF 㸬㞀ࡢࡓࡵ⏦ㄳ  ᖺ㛫ࡢ࠺ࡕ㸪 ᖺ༙௨ୖ࡟ࢃ

7SIOࡢᒙᗎᏛⓗ◊✲࡟ࡼࢀࡤ㸪ḟࡢࡼ࠺࡞࣐

ࡓࡗ࡚ᐇ㦂࡛ࡁ࡞࠸≧ἣࡀ⥆࠸࡚࠸ࡿ㸬ࡋࡓࢢ࣐άືࡀ᚟ඖࡉࢀ࡚࠸ࡿ㸦0DFKGD㸧㸬ࡀࡗ࡚㸪ᨺᑕ໬ศᯒ࡟㛵ࡍࡿෆᐜࢆ༑ศ࡟཯

᭱ึࡢᄇⅆ 7SIO$ ࡣ࣐ࢢ࣐㈏ධ࡟ࡼࡿ⃭ࡋ฼⏝᪋タ -55 7 ࣃ࢖ࣉࢥࣂࣝࢺ 60 ࣐࢞ࣥ⥺↷ᑕ᪋タ㸦㧗ᓮ㸧- 334 -

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56 ࡜ẚ㍑ࡋ㸪⣙  ಸࡢ 57/ ࢩࢢࢼࣝࡢ᳨

ࢧࣥࣉࣜࣥࢢヨᩱ࠿ࡽ௨ୗࡢᡭ㡰࡛▼ⱥࢆศฟ࡟ᡂຌࡋࡓ㸬ຍ⇕㏿ᗘࡣヨᩱࢆ☜ᐇ࡟ຍ⇕㞳ࡋࡓ㸬㟢㢌ࡢ῝ࡉ FP ࠿ࡽ᥇ྲྀࡉࢀࡓヨᩱࡉࡏࡿࡓࡵ㸪|&⛊ࡢ㐜࠸㏿ᗘ࡟タᐃࡋࡓ㸬ࡣ㸪ྵỈ⋡ ᐃᚋ㸪ỈὙࡋ㸪஝⇱ᚋ㸪̾

ࡲࡓ㸪ࢧࣥࣉࣝ࣍ࣝࢲ࣮࡜ 307 ࡢ㛫࡟ࣛ࢖ࢺȣP ࢧ࢖ࢬࡢ⢏Ꮚࢆศ㞳ࡍࡿࡓࡵ⠠࠸ศࡅࢆ࢞࢖ࢻࡀᤄධࡉࢀ㸪57/ ࢩࢢࢼࣝࡢ㏱㐣⬟ຊ⾜࡞ࡗࡓ㸬ḟ࡟ศ㞳⢏Ꮚࡢ໬Ꮫฎ⌮ࢆ㸪0ࢆྥୖࡉࡏ࡚࠸ࡿ㸬ࡲࡓ㸪ࣛ࢖ࢺ࢞࢖ࢻࡣࣄ

1D2+㸪0+&O㸪+) ࢆ⏝࠸࡚㸪ྛ  ᫬㛫㸪࣮ࢱ࣮ࡢ⇕࠿ࡽ 307 ࢆಖㆤࡍࡿᙺ┠ࢆᯝࡓࡋ࣐ࢢࢿࢸ࢕ࢵࢡࢫࢸ࢕࣮࣮ࣛ࡟ࡼࡿᨩᢾࢆ࠾

࡚࠸ࡿ㸬ࡇ࡞ࡗࡓ㸬ヨᩱࢆ஝⇱ᚋ㸪࢞ࣛࢫ㝖ཤࡢࡓࡵᐇ㦂࡛ࡣ㸪༢⢏Ꮚᐃ⏝ࡢヨᩱ࣍ࣝࢲ࣮ࢆ

ヨᩱࢆᣦ࡛⣽○ࡋ㸪⠠࠸ࢃࡅ࡟ࡼࡾ ̾

⏝ពࡋࡓ㸬᪂࣍ࣝࢲ࣮ࡣ┤ᚄ PP ࡢ㖟〇࡛㸪ȣP ⢏Ꮚ㑅ูࢆ⾜ࡗࡓ㸬ࡉࡽ࡟㸪 ᗘ┠ࡢ +)ࢭࣥࢱ࣮࡟┤ᚄ PP ࡢヨᩱಖᣢᏍࡀ࠶ࡾ㸪ฎ⌮ࢆ  ᫬㛫⾜࡞࠸㸪▼ⱥ⢏Ꮚࡢ⣧ᗘࢆ㧗ࡵᐃ⢏Ꮚࢆᤄධ࡛ࡁࡿ㸬ࡉࡽ࡟㸪㖟ࢧࣥࣉࣝ࣍

ࡿ࡜࡜ࡶ࡟㸪⢏Ꮚ⾲㠃ࡢ࢚ࢵࢳࣥࢢࢆ⾜࡞ࡗࣝࢲ࣮ࢆそ࠺㯮㞼ẕࢩ࣮ࣝࢻࡢ౑⏝࡟ࡼࡾ㸪ࡓ㸬᭱ᚋ࡟㸪⠠࠸ศࡅࢆ⾜࡞࠸㸪ᐇ㦂࡟⏝࠸ࣂࢵࢡࢢࣛ࢘ࣥࢻࢆࡉࡽ࡟పῶࡉࡏࡓ㸬ࡿ⢏ᚄ㸦ȣP㸧ࢆศ㞳ࡋࡓ㸬௨ୖࡢศ57/ ⿦⨨࡟ࡣᑠᆺ ; ⥺↷ᑕ⿦⨨ࡀᑟධࡉࢀ㸪㞳᪉ἲ࡟ࡼࡾ㸪ࢧࣥࣉࣜࣥࢢヨᩱ㸪.17.

6$5 ἲ*('UWG ࠿ࡽ ᐃ࡟ᚲせ࡞༑ศ࡞㔞ࡢ▼㠃࡟ࡣཌࡉ ȣP ࡢ࢔࣑ࣝࢩ࣮ࢺࡀᤄධࡉ

ⱥ⢏Ꮚࢆᚓࡿࡇ࡜ࡀ࡛ࡁࡓ㸬ࢀ㸪ప࢚ࢿࣝࢠ࣮ࡢ ; ⥺ࢆ㝖ཤࡋࡓᐃࡀྍ⬟࡛࠶ࡿ㸬ᑠᆺ ; ⥺⿦⨨ࡢ๓㸦+DVKLPRWRHWDO㸧㸬ࡑࡢ⤖ᯝ㸪:㸪

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JAEA-Review 2013-039

 ‶⁤⁦⁖•‧‟⁥․…

$ ࡛ *\PLQ ࡢᨺᑕ⥺ᙉᗘࢆ☜ಖࡍࡿࡇ㻟㻡㻜㻜࡜ࡀ࡛ࡁࡓ㻟㻜㻜㻜㻾㼀㻸 㼕㼚㼠㼑㼚㼟㼕㼠㼥6$5ἲ

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0XUUD\DQG:LQWOH  ࡟ࡼࡾᥦၐࡉࢀ㸪)DWWDKLDQG6WRNHV  ࡟ࡼࡗ࡚▼ⱥ57/ἲ࡟ึࡵ࡚ヨࡳࡽࢀࡓ6$5ἲࢆ㸪▼ⱥ༢⢏Ꮚ
57/ ᖺ௦ ᐃ࡟᥇⏝ࡋࡓ㸬

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▼ⱥࡢኳ↛ 57/ ᙉᗘࢆ ᐃᚋ㸪෌⌧ ; ⥺↷㻞㻜㻜ᑕࢆ *\ ࠶ࡿ࠸ࡣ *\ ࠿ࡽ *\ ࡲ࡛⾜࠸㸪㼀㼑㼙㼜㼑㼞㼍㼠㼡㼞㼑 㻔䉝㻕ࡑࢀࡒࢀࡢ 㸫|& 㛫ࡢ 57/

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Fig2㻌 ▼ⱥ༢⢏Ꮚ䛾Ⓨග᭤⥺ࢺ ᐃ㸦ࢸࢫࢺ↷ᑕ *\㸧ࢆ⾜࡞ࡗࡓ㸬ࣉࣞ

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ࣄ࣮ࢺ ᗘࡣ |&㸪 ⛊࡛⾜࡞ࡗࡓ㸬 ᐃࡢ᥎ዡ⃰ᗘࡣ㸪7K ࡀ  ࠿ࡽ SSP ࡢࡢ᭱ᚋ࡟ 'RVHUHFRYHU\WHVW㸦*\㸧ࢆ⾜⠊ᅖ㸪8 ࡀ  ࠿ࡽ SSP ࡢ⠊ᅖ࡟࠶ࡿ㸬࠸ 㸪 6$5 ᭤ ⥺ ࡢ ಙ 㢗 ᛶ ࢆ 5HF\FOLQJ UDWLRȚ⥺ᙉᗘ࡜᥎ዡ⃰ᗘ࠿ࡽᑟ࠿ࢀࡿ࢝ࣜࣈ࣮ࣞ

6$5'H*\ ࡟ࡼࡾ᳨ドࡋࡓ㸬▼ⱥ༢⢏Ꮚࢩࣙࣥ⥺ࢆ⏝࠸࡚㸪ᖺ௦ ᐃヨᩱࡢ 8 ࠾ࡼࡧࡢ 6$5

ᐃࡣヨᩱ .17.*(DQG'UWG

࠿ࡽᢳฟࡉࢀࡓ  ࠿ࡽ  ⢏Ꮚ࡟ࡘ࠸࡚⾜࡞

7K ⃰ᗘࡀỴᐃࡉࢀࡓ㸬ࡲࡓ㸪.2 ⃰ᗘࡣ ,&3࣐ࢫ࡟ࡼࡾỴᐃࡋࡓ㸬ࡗࡓ㸬ᐇ㦂⤖ᯝ࡜⪃ᐹⓎග᭤⥺࡜ࣉࣛࢺ࣮ࢸࢫࢺ

1$$ ศᯒヨᩱࡢᖺ㛫⥺㔞ࢆホ౯ࡍࡿࡓࡵ࡟㸪1$$ ἲ ᨵၿࡋࡓ

ᐃ⿦⨨ࢆ⏝࠸࡚⾜࡞ࡗࡓ▼ⱥ༢࡜,&3࣐ࢫἲ࡟ࡼࡾ*DQ]DZDHWDO  ࠾⢏Ꮚࡢ 6$5

ᐃࡢⓎග᭤⥺ࡢ୍౛㸦ヨᩱࢥ࣮ࡼࡧ*DQ]DZDDQG0DHGD  ࡢᡭ㡰࡟ᚑࡗࢻ㸸'UWGV㸧ࢆ )LJ ࡟♧ࡍ㸬ኳ↛57/࡚㸪87KDQG.2⃰ᗘࢆỴᐃࡋࡓ㸬ࡇࡢᙉᗘࡣ |& ࣆ࣮ࢡ௜㏆࡛⣙  ࢝࢘ࣥࢺࢆ

ࡘࡢᡭἲࡢෆ㸪1$$ࡣ 8࡜7Kࡢศᯒឤᗘ࡟ඃ♧ ࡋ 㸪 ෌ ⌧ ⥺ 㔞  5HJHQHUDWLYH GRVH ࢀࡿࡢ࡛㸪ཎᏊຊᶵᵓ࡟࠾࠸࡚ṇ☜࡞ྵ᭷㔞*\*\ ࡶ༑ศ࡟᫂░࡞Ⓨග࣮࢝ࣈ♧ࡋỴᐃࡢࡓࡵࡢヨ㦂ࢆ㐍ࡵ㸪᭱⤊ⓗ࡟ḟࡢᐃ࡚࠸ࡿ㸬ࡑࡇ࡛㸪ࣉࣛࢺ࣮㡿ᇦ࡟࠶ࡿ᪉ἲࢆ᥇⏝ࡋࡓ㸬୰ᛶᏊ↷ᑕࡣཎᏊຊᶵᵓ᪋

|& ࡢ |& 㛫ࡢ 57/ ✚⟬್ࢆ 57/ ᙉᗘタ-55ཎᏊ⅔㸪7ࣃ࢖ࣉ ᭱኱ฟຊ0:࡜ࡋࡓ )LJ ᤄධᅗ 㸬ࡲࡓ㸪ࢸࢫࢺࢻ࣮ࢬ

᭱኱୰ᛶᏊࣇ࢚ࣝࣥࢫ [ QFP V &Gᐃ࡟࠾࠸࡚ࡶྠࡌ ᗘ㡿ᇦࡢ 57/ ✚⟬್ࢆẚ ࡢ$࣏ࢪࢩ࡛ࣙࣥศ㛫⾜ࡗࡓ㸬↷ࢸࢫࢺࢻ࣮ࢬ 57/ ᙉᗘ࡜ࡋࡓ㸬ᑕヨᩱࡣ᫬㛫෭༷ࡋ㸪ࡑࡢᚋ㸪ඹྠ฼⏝኱Ꮫ㛤ᨺ◊✲ᐊ࡟タ⨨ࡉࢀࡓ$06ࡢ*Hࢹ࢕⵳✚⥺㔞࡜ᖺ㛫⥺㔞ࢸࢡࢱ࣮࡟ࡼࡾ㸪1S ࡛ࡣ NHY ࠾ࡼࡧ

6$5 ἲ ࡟ ࡼ ࡿ 'H ホ ౯ ࡢ ୍ ౛ 㸦 ヨ ᩱ 㸸NHY㸪 3D࡛ࡣNHYࡢȚ⥺ィ ࢆヨᩱ࡟

'UWGV㸧ࢆ )LJ ࡟♧ࡋࡓ㸬6$5 ⿵ṇ๓ᛂࡌ࡚ ࠿ࡽ ⛊㛫࠾ࡇ࡞ࡗࡓ㸬ࡢ⥺㔞ᛂ⟅⥺෌⌧⥺㔞*\㸫*\ 㛫࡛ࡼ࠸

ᐃヨᩱࡢ㔜㔞ࡣヨᩱ࠶ࡓࡾ࠿ࡽPJ┤⥺ᛶࢆ♧ࡍࡀ㸪ឤᗘኚ໬⋡࡟ᇶ࡙࠸࡚㸪ྛ

࡛1$$ ᐃࡣᅇ⾜࡞࠸㸪ࡑࡢᖹᆒ್ࢆ⃰ᗘ

57/

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ඖ57/ᙉᗘ㸧ࢆ⾜࡞ࡗࡓ㸬ࡑࡢ⤖ᯝ㸪ឤᗘ⿵ᐃ್ࡢឤᗘ⿵ṇ㸦↷ᑕ 57/ᙉᗘ⥺㔞᚟ᶆ‽ᒾ▼ヨᩱ࡜ࡋ࡚⏘ᴗᢏ⾡ᶵᵓ࠿ࡽᥦ౪

ṇ⥺㔞ᛂ⟅⥺ࡢഴࡁࡣࡸࡸῶᑡࡋ㸪ヨᩱࡢ 'H

ࡉࢀࡓ  ヨᩱࢆ⏝࠸ࡓࡀ㸪ࡑࢀࡽ  ࡘࡢ᰾✀ࡣឤᗘ⿵ṇ๓ࡢ *\ ࠿ࡽ *\ ࡟ቑຍࡋࡓ㸬

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JAEA-Review 2013-039‶⁤⁦⁖•‧‟⁥․…

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3UHVFRWW DQG 6WHSKDQ

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3UHVFRWWDQG+XWWRQ  ࡀ♧ࡋࡓ㸪໭⦋⁊‟⁤⁓⁫ ⁖⁡⁥⁗‣‫⁫‹ ‧‫‬

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⪃࡟ࡋࡓ㸬ࡇࡢ್ࢆࢧࣥࣉࣜࣥࢢᆅⅬࡢ㧗ᗘ࡜῝ᗘ࠿ࡽᰝᐃࡋࡓ⤖ᯝ㸪Ᏹᐂ⥺㔞ࡣࢃࡎ࠿
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௨ୖࡢᨺᑕᛶඖ⣲⃰ᗘ㸪ș⥺㏱㐣⋡࠾ࡼࡧྵ⁄⁗⁕⁡⁨⁗⁤⁫ ‶⁗‣‫⁫‹ …‫‬

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Ỉ⋡࠿ࡽᑟ࠿ࢀࡿᖺ㛫⥺㔞࡜Ᏹᐂ⥺㔞㸦 ࠿ࡽ  P*\D 㸧 ࡢ ྜ ィ ࠿ ࡽ ᚓ ࡽ ࢀ ࡿ 'D㻾㼍㼐㼕㼍㼠㼕㼛㼚 㼐㼛㼟㼑 㻔㻳㼥㻕㸦 .1 㸪 *( 㸪 7. 㸪'UWG ⥺㔞ᛂ⟅᭤⥺䛸▼ⱥ䛾SAR䛻䜘䜛ឤᗘኚ໬
Fig.3

㸻P*\D㸧ࢆ 7DEOH ࡟♧ࡋࡓ㸬ࡲࡓ㸪⥺㔞᚟ඖࢸࢫࢺ࡛ࡣ㸪᪤▱↷ᑕ㔞 ▼ⱥ༢⢏Ꮚ 57/ ᖺ௦*\ ࡟ᑐࡋ㸪ឤᗘ⿵ṇ᚟ඖ 'H ࡣ *\ ࢆ♧᭱ึᮇⅆ○ὶ 7SIO$ .1 ࡢ  ⢏Ꮚࡢ 6$5ࡋ㸪⥺㔞᚟ඖ⋡ࡣ 㸦㸻*\*\㸧ࡢࡼ࠸್ࢆ♧ࡋࡓ㸬ࡇࡢ⤖ᯝࡣ㸪ᐇ㦂࡛⏝࠸ࡓᖺ௦ࡢⅆᒣ▼ⱥࡢ 'H Ỵᐃ࡟ 6$5 ἲࡀ㐺ࡋ࡚࠸ࡿࡇ࡜ࡍࡿ  ⢏Ꮚ࡜኱ࡁࡃࡣࡎࢀࡿ  ⢏ᏊࡀᏑᅾࢆ♧ࡋ࡚࠸ࡿ㸬ࡋࡓࡀࡗ࡚㸪ᮏᐇ㦂࡛ࡣࡍ࡭ࡋࡓ㸬 ⢏Ꮚࢆ㝖እࡋࡓ  ⢏Ꮚࡢ 6$5 ᖺ௦ᐃㄗᕪࡀ Ȫෆ࡟ศᕸࡣ ND ࡢ⠊ᅖࢆ♧ࡍ㸬57/

࡚ࡢ▼ⱥ༢⢏Ꮚ࡛ 6$5'H Ỵᐃ࡜⥺㔞᚟ඖࢸࢫࢺ࡟ࡼࡾ⥺㔞ᛂ⟅⥺ࡢಙ㢗ᛶࢆホ౯ࡋࡓ㸬

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⁓

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- 337 -

3-6

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JAEA-Review 2013-039


Table 1 Ὕ√ⅆ○ὶ▼ⱥ༢⢏Ꮚ䛻䜘䜛SARᖺ௦㻲㼘㼛㼣㻌㼡㼚㼕㼠㼀㼜㼒㼘㻌㻭
㼀㼜㼒㼘㻌㻮
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㻿㼍㼙㼜㼘㼑 㻳㼞㼍㼕㼚㼏㼛㼐㼑 㼚㼡㼙㼎㼑㼞
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㻾㼑㼏㼥㼏㼘㼕㼚㼓㻚㻌㼞㼍㼠㼕㼛㻭㼢㼑㻚㻌㻔㻾㼍㼚㼓㼑㻕㻝㻚㻜㻝㻌㻔㻜㻚㻥㻞㻙㻝㻚㻝㻜㻕㻝㻚㻜㻜㻌㻔㻜㻚㻤㻤㻙㻝㻚㻞㻜㻕㻜㻚㻥㻢㻌㻔㻜㻚㻣㻠㻙㻝㻚㻜㻤㻕㻝㻚㻝㻡㻌㻔㻜㻚㻢㻟㻙㻝㻚㻞㻝㻕䃦㻞㻌㼠㼑㼟㼠 㻻㼠㼔㼑㼞㼟㻔㻑㻕㻠㻢㻚㻤㻰㼑㼠㼞㼕㼠㼡㼟
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࠾ࡼࡧᖺ㛫⥺㔞ㄗᕪࢆ⪃៖ࡋࡓᖹᆒᖺ௦ࡣLVRWKHUPDOUHGWKHUPROXPLQHVFHQFH ,57/ sND ࡜࡞ࡗࡓ 7DEOH 㸬7SIO% ⅆ○ὶ

GDWLQJRIYROFDQLFXVLQJWKH6$5PHWKRG

*( ࠾ࡼࡧ 7. ࡢ༢⢏Ꮚᖺ௦ࡣࡑࢀࡒࢀ㸪

5DGLDW0HDV

ND㸪ND ࡢศᕸࢆ♧ࡋ㸪ㄗᕪࢆ⪃+DVKLPRWR7+DEXNL+7DQDEH,៖ࡋࡓᖹᆒᖺ௦ࡣ sND㸪sND ࡛࠶

6DNDL77DNDKDVKL6'DWLQJࡿ㸬7SIO& ⅆ○ὶ 'UWG ࡢ༢⢏Ꮚᖺ௦ࡣ㸪XVLQJUHGWKHUPROXPLQHVFHQFHIURPTXDUW]

ND ࡢࡸࡸᗈ࠸⠊ᅖ࡟࠶ࡾ㸪ᖹᆒᖺ௦ࡣJUDLQVLQVWUDWDUHODWHGWRIRVVLOERQHVRI

sND ࡛࠶ࡿ㸬(OHSKDV1DXPDQQL&KLN\XNDJDNX

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+DVKLPRWR71DNDJDZD7+RQJ'*࠶ࡾ㸪ⅆ○ὶࡀ㐃⥆ⓗ࡛▷ᮇ㛫࡟ᄇⅆࡋࡓࡇ

7DNDQR0$QDXWRPDWHGV\VWHPIRU

࡜ࢆ♧ࡋ࡚࠸ࡿ㸬ࡇࢀࡽࡢᖺ௦ࡣᆅ㉁Ꮫ᥎ᐃ

ERWKUHGEOXHWKHUPROXPLQHVFHQFHDQG

ᖺ௦࡜ࡼࡃ୍⮴ࡋࡓ㸬ࡇࡢ⤖ᯝࡣ㸪ᮏㄽ࡛㐍

RSWLFDOO\VWLPXODWHGOXPLQHVFHQFHࡵࡓ༢⢏Ꮚ▼ⱥ࡟ࡼࡿ 57/6$5 ἲࡣⅆ○ὶሁ

PHDVXUHPHQWV-1XFO6FL7HFKQRO

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UHGWKHUPROXPLQHVFHQFH 57/ VWXGLHVRQᩥ⊩

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)DWWDKL06WRNHV6([WHQGLQJPDNHUWHSKUDVLQDQGDURXQG-DSDQ*OREDO

WKHWLPHUDQJHRIOXPLQHVFHQFHGDWLQJXVLQJ

DQG3ODQHWDU\&KDQJH

7/ 57/ IURPYROFDQLFTXDUW]5DGLDW0HDV0DFKLGD+$UDL)$WODVRI



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)DWWDKL06WRNHV6'DWLQJ

7RN\R3UHVV7RN\R LQ-DSDQHVH 

XQKHDWHGTXDUW]XVLQJDVLQJOHDOLTXRW

0LDOOLHU')DLQ-0RQWUHW0

UHJHQHUDWLRQGRVHUHGWKHUPROXPLQHVFHQFH

3LOOH\UH76DQ]HOOH66RXPDQD6

SURWRFRO 6$557/ -RXUQDORI3URSHUWLHVRIWKHUHG7/SHDNRI/XPLQHVFHQFHTXDUW]UHOHYDQWWRWKHUPROXPLQHVFHQFH

*DQ]DZD<)XUXNDZD++DVKLPRWR7

GDWLQJ1XFO7UDFNV5DGLDW0HDV  

6DQ]HOOH60LDOOLHU'3LOOH\UH7

6LQJOHJUDLQVGDWLQJRIYROFDQLF

0LDOOLHU')DLQ-0RQWUHW0

TXDUW]IURPS\URFODVWLFIORZVXVLQJ5HG7/

3LOOH\UH76DQ]HOOH66RXPDQD6

5DGLDW0HDV

6XQEOHDFKLQJRIWKHUHG7/RITXDUW]

*DQ]DZD<0DHGD0|&

SUHOLPLQDU\REVHUYDWLRQV$QFLHQW7/

3-6- 338 -

㻥㻡

JAEA-Review 2013-039



 5HG,7/ GDWLQJ RI YROFDQLF TXDUW]

0XUUD\$6:LQWOH$*JUDLQV XVLQJ RYHU  Υ  VLJQDOV WK/XPLQHVFHQFHGDWLQJRITXDUW]XVLQJDQLQWHUQDWLRQDO

LPSURYHGVLQJOHDOLTXRWUHJHQHUDWLYHGRVH

OXPLQHVFHQFHDQGHOHFWURQVSLQUHVRQDQFH

SURWRFRO5DGLDW0HDVGDWLQJ 㻞㻜㻜㻤㻚㻌 㻥㻚㻌 㻝㻤㻚 㻌 㻼㼑㼗㼕㼚㼓㻌 㼁㼚㼕㼢㼑㼞㼟㼕㼠㼥㻚㻌

6WRNHV6)DWWDKL05HGHPLVVLRQ㻯㼔㼍㼚㼕㼍㻚OXPLQHVFHQFHIURPTXDUW]DQGIHOGVSDUIRU

 'DWLQJWKHDFWLYLW\RI7R\DFDOGHUDGDWLQJDSSOLFDWLRQVDQRYHUYLHZ5DGLDW-DSDQXVLQJVLQJOHJUDLQVE\PHDQVRIUHG

0HDVWKHUPROXPLQHVFHQFH 6$5 GDWLQJWK

3UHVFRWW-56WHSKDQ/*7KH

-DSDQ.RUHD&KLQDLQWHUQDWLRQDOZRUNVKRSFRQWULEXWLRQRIFRVPLFUDGLDWLRQWRWKH

RQSUHVHQWHDUWKVXUIDFHSURFHVVDQG

HQYLURQPHQWDOGRVHIRUWKHUPROXPLQHVFHQFHKLVWRULFDOHQYLURQPHQWDOFKDQJHVLQ(DVWGDWLQJ3$&7

$VLD+DNRGDWH

3UHVFRWW-5+XWWRQ-7&RVPLF

 6$55HG7/GDULQJRIODWH3OHLVWRFHQH

UD\FRQWULEXWLRQVWRGRVHUDWHVIRU

7R\DYROFDQR-DSDQ8VLQJVLQJOHTXDUW]

OXPLQHVFHQFHDQG(65GDWLQJODUJHGHSWKVJUDLQVQG$VLD3DFLILF&RQIHUHQFHRQ

DQGORQJWHUPWLPHYDULDWLRQV5DGLDWOXPLQHVFHQFHDQG(65GDWLQJ

0HDV

$KPHGDEDG,QGLD<DZDWD7

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IRUVLQJOHJUDLQTXDUW]5DGLDW0HDV

 6$5 ἲ࡟ࡼࡿὝ√ⅆ○ὶሁ✚≀ࡢ㉥Ⰽ⇕ࣝ

࣑ࢿࢭࣥࢫᖺ௦ᐃ 㬎⃝ዲ༤㸪⮻஭⌮Ἃ㸪⏣୰▖㸪ᮾ๛㸪ᆅ㉁Ꮫ㞧ㄅ㸪㸪㸦㸧ᡂᯝࡢබ⾲



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<DPDPRWR . .DVKLZD\D < *DQ]DZDᰩ⏣ᐶᏊ㸪⣽⏿᭷ᮍ㸪 ᖺᗘ᪥ᮏᆅ㉁Ꮫ

&KHPLFDO *HRORJ\ 9ROXPH  ,VVXH ఍  ᖺḟ⥲఍㸪ᮐᖠ3DJHV   ⅆᒣ▼ⱥ༢⢏Ꮚࡢ 5HG7/㸫6$5 ᖺ௦ ᐃ㸬㬎⃝ዲ༤㸪ụ㯞⏤⨾㸪 ᖺᗘ࣑ࣝࢿࢭࣥGDWLQJ WHUUDFH GHSRVLWV XVLQJ UHGࢫᖺ௦ ᐃ◊✲఍㸪㸬㸬ዉⰋዪᏊ኱ᏛWKHUPROXPLQHVFHQFHIURPTXDUW]<*DQ]DZD 6$5 ἲ࡟ࡼࡿ 5HG7/㸫Υ,7/ ᖺ௦ ᐃ㸬

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/$,&306 DQDO\VLV RI SUHVVHG SRZGHU

6LQJOHJUDLQWZRIUDJPHQWPHWKRGIRU ᖺ௦ ᐃ◊✲఍㸪㸬㸬ዉⰋዪᏊ኱Ꮫ

 ࣂ࢖࢝ࣝ†⣽⢏ሁ✚≀ࡢ࣑ࣝࢿࢵࢭࣥࢫWKHUPROXPLQHVFHQFHᖺ௦ᐃ㸬ఀ⸨୍඘㸪㛗㇂㒊ᚨᏊ㸪㬎⃝ዲ

YROFDQLF TXDUW] XVLQJ 6$5 PHWKRG <༤㸪᯽㇂೺஧㸪 ᖺᗘ࣑ࣝࢿࢭࣥࢫᖺ௦

*DQ]DZD00DHGD5DGLDWLRQ0HDVXUHPHQWVᐃ◊✲఍㸪㸬㸬ዉⰋዪᏊ኱Ꮫ

Υ

LVRWKHUPDO

,57/  GDWLQJ RI

9ROXPH  - 339 -

UHG

3-6

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JAEA-Review 2013-039

3-7
㺀℩ᡞෆⅆᒣᒾ㢮୰ࡢࣄ⣲㸪࢔ࣥࢳࣔࣥྵ᭷㔞㺁
$UVHQLFDQGDQWLPRQ\FRQWHQWVLQWKH6HWRXFKL9ROFDQLF5RFNVᮾி⤒῭኱Ꮫ࣭⤒ႠᏛ㒊࣭᪂ṇ⿱ᑦ+LURQDR6KLQMRH )DFXOW\RI%XVLQHVV$GPLQLVWUDWLRQ7RN\R.HL]DL8QLYHUVLW\ 㸦㸯㸧 ◊✲ࡢ┠ⓗ࡜ព⩏ ᓥᘼⅆᒣᒾࡢ࣐ࢢ࣐ᡂᅉࢆ⪃࠼ࡿୖ࡛㸪ỿࡳ㎸ࡴࢫࣛࣈ࡟⏤᮶ࡍࡿᡂศࡢホ౯ࡣᴟࡵ࡚㔜せ࡛࠶ࡿ㸬ࡲࡓ㸪ࡑࡢࢫࣛࣈ⏤᮶ᡂศࢆ࣐ࣥࢺ࢙ࣝ࢘ࢵࢪ࡟ࡶ
ࡓࡽࡍ፹యࡣ㸪Ỉࢆ୰ᚰ࡜ࡍࡿὶయ┦࡛࠶ࡿࡢ࠿㸪ࢣ࢖㓟ሷ࣓ࣝࢺ࡛࠶ࡿࡢ࠿ࡶ㔜せ࡞ၥ㢟ࡢ୍ࡘ࡛࠶
ࡿ㸬ỿࡳ㎸ࡴࢫࣛࣈࡢ ᗘᵓ㐀࡟ࡼࡾ㸪୧⪅ࡢ࠸ࡎࢀࡀ୺య࡜࡞ࡿ࠿ࡀỴࡲࡾ㸪ᓥᘼ࡟ࡼࡾ㸪ࡉࡽ࡟ᓥᘼࡢ୰࡛ࡶ␗࡞ࡿࡶࡢ࡜ぢࡽࢀࡿ㸬 ୍⯡࡟㸪ᾏᕊỿࡳ㎸ࡳࡢぢࡽࢀࡿࡼ࠺࡞㸪㧗 ࡢᾏὒࣉ࣮ࣞࢺỿࡳ㎸ࡳࡀ࠾ࡇࡗࡓሙᡤ࡟࠾࠸࡚ࡣ㸪ࢫࣛࣈ⏤᮶ᡂศࡀ㸪୺࡟ࢣ࢖㓟ሷ࣓ࣝࢺ࡜ࡋ࡚ࠊ࣐
ࣥࢺ࢙ࣝ࢘ࢵࢪ࡟ῧຍࡉࢀࡿࡶࡢ࡜ࡉࢀࡿ㸬ࡍ࡞ࢃࡕ㸪ỿࡳ㎸ࡴࢫࣛࣈࡀ⼥ゎࡋ࡚Ⓨ⏕ࡋࡓ࣓ࣝࢺࡀୖ
఩ࡢ࣐ࣥࢺ࢙ࣝ࢘ࢵࢪࢆởᰁࡍࡿ㸬 ࡇࡢࡼ࠺࡞ࢫࣛࣈ⏤᮶ᡂศࡢホ౯ࡣ㸪࠸ࢃࡺࡿᾮ
┦⃰㞟ඖ⣲㸦LQFRPSDWLEOHHOHPHQW㸧ࡢྵ᭷㔞ࡸ✀ࠎࡢྠ఩య⤌ᡂ㸦6U1G3E ➼㸧ࡢศᯒ࡟ᇶ࡙࠸࡚⾜ࢃࢀࡿࡇ࡜ࡀከ࠸㸬ࡇࢀࡽࡢඖ⣲⃰ᗘࡣ㸪⤖ᬗศ໬స⏝➼㸪ὸᡤ࡛ࡢ࣐ࢢ࣐㐍໬ࣉࣟࢭࢫ࡛ࡶኚ໬ࡍࡿ㸬ࡲࡓ㸪ᓥᘼ࣐ࢢ࣐ࡢሙྜ㸪ཌ࠸ᆅẆࢆ㏻㐣ࡍࡿ㝿ࡢ㸪ᆅẆ≀㉁ࡢྠ໬ࡸΰᰁࡶホ౯ࡢጉࡆ࡟࡞ࡿ㸬ࡑࡇ࡛㸪
グ㍕ᒾ▼Ꮫⓗ࡟࡞ࡿ࡭ࡃᮍศ໬࡞ᒾ▼࡜ุ᩿ࡉࢀࡿ
ࡶࡢࢆヨᩱ࡜ࡋ࡚⏝࠸ࡿࡇ࡜ࡀᮃࡲࡋ࠸㸬ࡲࡓ㸪ඖ⣲✀࡟ࡼࡾὶయ┦ࡸ㸪ࢣ࢖㓟ሷ࣓ࣝࢺࡢ୰࡛ࡢᣲື
ࡀ␗࡞ࡿࡢ࡛㸪ᵝࠎ࡞ඖ⣲✀㸪࠶ࡿ࠸ࡣྠ఩య✀ࡢศᯒ࡟ࡼࡾᚓࡽࢀࡿ᝟ሗࢆ⥲ྜⓗ࡟᳨ウࡍࡿࡇ࡜ࡀ
ᮃࡲࡋ࠸㸬 ୖグࡢࡼ࠺࡞㸪ᓥᘼ࣐ࢢ࣐࡬ࡢࢫࣛࣈ⏤᮶ᡂศࡢ㈉⊩ࡢホ౯ࢆ⾜࠺ᑐ㇟ࡢ୍౛࡜ࡋ࡚㸪௒ᅇࡣす༡᪥ᮏᘼ࡛୰᪂ୡ୰ᮇ࡟άືࡋࡓ℩ᡞෆⅆᒣᒾࡢ㧗 0JᏳᒣᒾ࠾ࡼࡧ⋞Ṋᒾ୰ࡢࣄ⣲㸪࢔ࣥࢳࣔࣥྵ᭷㔞ࡢ୰ᛶᏊᨺᑕ໬ศᯒࡢ⤖ᯝࢆሗ࿌ࡍࡿ㸬ࡑࡢព⩏࡜ࡋ࡚ࡣ㸪௨ୗ࡟ᥖࡆࡿࡼ࠺࡞ࡶࡢࡀ࠶ࡿ㸬D ℩ᡞෆⅆᒣᒾࡣ᪥ᮏᾏᙧᡂ࡟క࠺㸪す༡᪥ᮏᘼࡢ
᫬ィᅇࡾᅇ㌿┤ᚋࡢ㸪㧗 ࡢᅄᅜᾏ┅ࢫࣛࣈࡢỿ
ࡳ㎸ࡳࡢࡶ࡜࡛άືࡋࡓࡶࡢ࡛࠶ࡿ㸬E ℩ᡞෆⅆᒣᒾࡢ࡞࠿࡛㸪⋞Ṋᒾ࠾ࡼࡧ㸪㧗 0J Ᏻᒣᒾ࣐ࢢ࣐ࡣグ㍕ᒾ▼Ꮫⓗ≉ᚩ࠿ࡽ㸪࣐ࣥࢺࣝ࢘
࢙ࢵࢪ࠿ࢇࡽࢇᒾ࡜ᖹ⾮࡟Ꮡᅾࡋᚓࡓ㸪ึ⏕ⓗ࣐ࢢ࣐࡛࠶ࡿ㸬F ℩ᡞෆⅆᒣᒾ㢮ࡢ⋞Ṋᒾ࠾ࡼࡧ㸪㧗 0J Ᏻᒣᒾ࡟ࡘ࠸࡚ࡣ㸪ࢫࣛࣈ⼥ゎ࣓ࣝࢺ࡜࣐ࣥࢺ࢙ࣝ࢘ࢵࢪ
ࡢ཯ᛂ࡟ࡼࡿ࣐ࢢ࣐ᡂᅉࡀᥦ᱌ࡉࢀ㸪ከ✀ࡢᾮ┦⃰㞟ඖ⣲ࡸྠ఩య✀ࢆྲྀࡾධࢀࡓ㸪ࡑࡢ࣐ࢢ࣐ᡂ
ᅉㄽ࡟ἢࡗࡓࣔࢹࣝࡀ᳨ウࡉࢀ࡚࠸ࡿ㸬ࡋ࠿ࡋࡇࢀࡲ࡛㸪ぶ㖡ඖ⣲࡛࠶ࡿࣄ⣲ࡸ࢔ࣥࢳࣔࣥ࡟ࡘ࠸
࡚ࡢศᯒࡢሗ࿌ࡣ↓࠸㸬ࡇࢀࡽࡢඖ⣲ࡣ㸪ỿࡳ㎸ࡴࢫࣛࣈୖࡢሁ✚≀ࡸ⇕Ỉኚ㉁ࢆཷࡅࡓ⋞Ṋᒾ࡟ࡣ㇏ᐩ࡟ྵࡲࢀ㸪ࢫࣛࣈ⏤᮶ᡂศࡢホ౯࡟ࡣ㸪㔜せ࡞ඖ⣲✀ࡢ୍ࡘ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡿ㸬ẚ㍑ྍ
⬟࡞✀ࠎࡢᆅ⌫໬Ꮫⓗࢹ࣮ࢱࡢ⵳✚ࡉࢀ࡚࠸ࡿ㸪℩ᡞෆⅆᒣᒾ㢮ࡢ⋞Ṋᒾ࠾ࡼࡧ㸪㧗 0J Ᏻᒣᒾ࡟ࡘ࠸࡚ࡢศᯒࢆ⾜࡞࠺ࡇ࡜࡛㸪ぶ㖡ඖ⣲ࢆྵࡵ࡚㸪ࢫࣛࣈ⏤᮶ᡂศࢆ⥲ྜⓗ࡟᳨ウࡍࡿࡇ࡜ࡀ࡛ࡁ
ࡿ࠿ࡶࡋࢀ࡞࠸㸬G ࣄ⣲ࡸ࢔ࣥࢳࣔࣥࡣ㠀◚ቯࡢ୰ᛶᏊᨺᑕ໬ศᯒ
࡟ࡼࡾ㸪௚ࡢᡭἲࡼࡾ㸪ẚ㍑ⓗ⢭ᗘࡼࡃᐃ㔞ࡍࡿࡇ࡜ࡀ࡛ࡁࡿ㸬 ࡞࠾㸪ᮏ◊✲࡟⏝࠸ࡓヨᩱ࡟ࡘ࠸࡚ࡣᚋ㏙ࡍࡿࡼ࠺࡟㸪ࣄ⣲㸪࢔ࣥࢳࣔࣥࡢࡳ࡞ࡽࡎ✀ࠎࡢᚤ㔞ඖ⣲⃰ᗘࡢศᯒࡶేࡏ࡚⾜ࡗ࡚࠸ࡿ㸬㔝እㄪᰝࡸヨᩱࡢධᡭ࠾ࡼࡧ㸪୰ᛶᏊᨺᑕ໬ศᯒ௨እࡢศᯒ࡟ࡘ࠸࡚
ࡣ㸪⏘ᴗᢏ⾡⥲ྜ◊✲ᡤࡢゅ஭ᮅ᫛Ặ࠾ࡼࡧ㸪ᮾி኱Ꮫᆅ㟈◊✲ᡤࡢᢡᶫ⿱஧Ặ࡜ࡢඹྠ◊✲࡜ࡋ࡚⾜ࢃࢀࡓࡶࡢ࡛࠶ࡿ㸬ࡲࡓᚋ㏙ࡢ⺯ග㹖⥺ศᯒ࠾ࡼࡧ㸪,&306 ศᯒࡣᮾி኱Ꮫᆅ㟈◊✲ᡤࡢඹྠ฼⏝ࣉࣟࢢ࣒ࣛࡢ᥼ຓࢆཷࡅ࡚⾜ࡗࡓࡶࡢ࡛࠶ࡿ㸬㸦㸰㸧 ◊✲᪉ἲ ヨᩱࡣ㸪஑ᕞ㹼⣖ఀ༙ᓥす㒊ࡢ℩ᡞෆⅆᒣᒾศᕸᇦࡢྛᆅ࠿ࡽ㸪㧗 0J Ᏻᒣᒾ࠾ࡼࡧ㸪⋞Ṋᒾࢆ཰㞟ࡋࡓ㸬ิᣲࡍࡿ࡜㸪኱ศ┴ࡢ኱㔝ⅆᒣᒾ㢮㸪ឡ፾┴ࡢ㧗⦖༙ᓥ࿘㎶㸪㤶ᕝ┴ࡢㆭᒱᖹ㔝࠾ࡼࡧᑠ㇋ᓥ㸪኱

JRR-4 T, S ࣃ࢖ࣉ ᆅ⌫⛉Ꮫヨᩱᨺᑕ໬ศᯒ

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JAEA-Review 2013-039

ࠥSSP㸪࢔ࣥࢳࣔࣥࡢྵ᭷㔞ࡣ㸪ࠥSSP
࡛࠶ࡗࡓ㸬⋞Ṋᒾ࡟ࡘ࠸࡚ࡣ㸪ࣄ⣲ࡢྵ᭷㔞ࡣ ࠥSSP㸪࢔ࣥࢳࣔࣥࡢྵ᭷㔞ࡣ ࠥSSP ࡛࠶ࡗࡓ㸬ศᯒ⤖ᯝࡢ౛ࢆ⾲㸯࡟ᥖࡆࡿ㸬ඛ࡟㏙࡭ࡓ
ࡼ࠺࡟㸪ヨᩱࡣᓥᘼఙ㛗㸦ᮾす㸧᪉ྥ࡟ᩘᆅᇦ࠿ࡽ
཰㞟ࡋࡓࡶࡢ࡛࠶ࡿࡀ㸪ࣄ⣲㸪࢔ࣥࢳࣔࣥྵ᭷㔞࡟ࡘ࠸࡚㸪ᮾす᪉ྥࡢኚ໬ഴྥࡣぢࡽࢀ࡞࠿ࡗࡓ㸬 ࣐ࢢ࣐ᄇฟ๓ࡢ⤖ᬗศูࡸ㸪࣐ࣥࢺ࡛ࣝࡢ࣐ࢢ࣐
ศ㞳᫬ࡢ㒊ศ⼥ゎᗘࡢຠᯝࢆ࢟ࣕࣥࢭࣝࡍࡿࡓࡵ࡟㸪┦஫࡟࣐ࣥࢺࣝ㖔≀࡟ᑐࡍࡿᾮ┦⃰㞟ᗘࡢ㢮ఝࡋࡓඖ⣲ࡢẚࢆྲྀࡿࡇ࡜ࡀ࠶ࡿ㸬ࣄ⣲ࡸ࢔ࣥࢳࣔࣥࡢᾮ
┦⃰㞟ᗘ࡟ࡘ࠸࡚ࡣ㸪㈨ᩱࡀஈࡋ࠸ࡀ &H ࡜ẚ㍑ⓗᾮ┦⃰㞟ᗘࡀ㏆࠸࡜ࡍࡿ 1ROOHWDO  ࡟ᚑ࠸㸪
$V&H6E&H ẚ࡟ࡘ࠸᳨࡚ウࡍࡿ㸬㜰ᆅᇦ࡛࠶ࡿ㸬⢒๭ࡋࡓᒾ▼∦ࢆὙίᚋ㸪࣓ࣀ࢘⮬ືங㖊࡛⣽⢊໬ࡋࡓࡶࡢࢆศᯒ࡟౪ࡋࡓ㸬℩ᡞෆⅆᒣᒾ㢮ࡣྂ඾ⓗ࡟ࡣ㸪ᮾࡣឡ▱┴ࡢタᴦᆅᇦ࠿ࡽ㸪すࡣ஑ᕞᮾ㒊ࡢ኱㔝ⅆᒣᒾ㢮ࡲ࡛ࡢศᕸᇦ
ࢆᣢࡘ࡜ࡉࢀࡿ㸬ࡋ࠿ࡋ㸪℩ᡞෆⅆᒣᒾ㢮ࢆ≉ᚩ࡙ࡅࡿ㸪㧗 0J Ᏻᒣᒾࡀฟ⌧ࡍࡿࡢࡣ㸪௒ᅇศᯒࡋ
ࡓヨᩱࢆㄪ㐩ࡋࡓ஑ᕞ㹼⣖ఀ༙ᓥす㒊ࡢ⠊ᅖ࡟㝈ࡽࢀࡿ ᅗ㸯㸸℩ᡞෆⅆᒣᒾ㢮ࢆྵࡴ㸪୰ᮇ୰᪂ୡࡢす༡᪥ᮏᘼࡢᾏ⁁ᐤࡾⅆᡂᒾࡢศᕸ
 ୰ᛶᏊᨺᑕ໬ศᯒࢆ⾜࡞ࡗࡓヨᩱ࡟ࡘ࠸࡚ࡣ㸪ྜࢃࡏ࡚㸪⺯ග ; ⥺ศᯒ࡟ࡼࡾ㸪୺ᡂศ࡜୍㒊ࡢᚤ㔞ඖ⣲⤌ᡂࢆᐃ㔞ࡋ㸪ࡉࡽ࡟ ,&306 ࢆ⏝࠸࡚㸪ᕼᅵ㢮ඖ⣲ࢆྵࡴከࡃࡢᚤ㔞ඖ⣲⤌ᡂࢆᐃ㔞ࡋࡓ㸬ࡲࡓ㸪ᮏሗ࿌࡛ࡣྲྀࡾᢅࢃ࡞࠸ࡀ㸪-55 ཎᏊ⅔
࡟ᩜタࡢ⇕୰ᛶᏊࣅ࣮࣒ࣛ࢖࡛ࣥࡢ༶Ⓨ࣐࢞ࣥ⥺ศᯒ࡟ࡼࡾ㸪࣍࢘⣲ྵ᭷㔞ࡢᐃ㔞ࡶేࡏ࡚⾜ࡗ࡚࠸ࡿ㸬 ࣄ⣲㸪࢔ࣥࢳࣔࣥࡢᐃ㔞ࡣ᪥ᮏཎᏊຊ◊✲㛤Ⓨᶵᵓᮾᾏ◊✲㛤Ⓨࢭࣥࢱ࣮ࡢ -55 ཎᏊ⅔ࢆ⏝࠸ࡓ୰ᛶᏊᨺᑕ໬ศᯒ࡛⾜ࡗࡓ㸬࡞࠾㸪ࡇࢀࡽࡢඖ
⣲ࢆࡼࡾ⢭ᗘࡼࡃᐃ㔞ࡍࡿࡓࡵ࡟㸪ヨᩱࢆ࢝ࢻ࣑
࣒࢘ᯈ࡛ໟࡴࡇ࡜࡟ࡼࡾ㸪୺࡟⇕እ୰ᛶᏊࡢ↷ᑕ࡟ࡼࡿᨺᑕ໬ࢆ⾜ࡗࡓ㸬 ⢊ᮎヨᩱࡣ࣏࢚ࣜࢳࣞࣥ⿄࡟㸰㔜࡟⼥ᑒࡋࡓᚋ㸪 ヨᩱ࠶ࡲࡾࢆ࡜ࡾࡲ࡜ࡵ࡚㸪࢝ࢻ࣑࣒࢘ᯈ࡛඲యࢆそࡗࡓ㸬ࡉࡽ࡟ࡑࢀࢆཌᡭࡢ࣏࢚ࣜࢳࣞࣥ⿄ෆ࡟⼥ᑒࡋࡓࡶࡢࢆ㸪↷ᑕ⏝ࡢヨᩱ࡜ࡋࡓ㸬↷ᑕࡣ㸪-55 ཎᏊ⅔ࡢపฟຊ㸦N:㸧㐠㌿᫬࡟㸪7
ࡲࡓࡣ 6 ࣃ࢖ࣉ࡟࠾࠸࡚㸪 ศ㛫⾜ࡗࡓ㸬ࡑࡢᚋ ᪥㛫෭༷ࡋ㸪኱Ꮫ㛤ᨺ◊✲ᐊࡢ࣐࢞ࣥ⥺ࢫ࣌ࢡࢺ࣓࣮ࣟࢱ࣮㸦$6&㸧࡛࣐࢞ࣥ⥺ィ ࢆ⾜ࡗࡓ㸬ᐃ㔞ࡣ㸪⏘ᴗᢏ⾡⥲ྜ◊✲ᡤ㸪ᆅ㉁ㄪᰝ⥲ྜࢭࣥࢱ࣮ࡢᆅ⌫໬Ꮫ㸦ᒾ▼㸧ᶆ‽ヨᩱ࡛࠶ࡿ -$ ࢆᶆ‽࡜ࡋ࡚ᑐẚἲ࡛⾜ࡗࡓ㸦㸱㸧⤖ᯝ࡜㆟ㄽ  㧗 0J Ᏻᒣᒾ࡟ࡘ࠸࡚ࡣ㸪ࣄ⣲ࡢྵ᭷㔞ࡣ㸪ᅗ 㸸℩ᡞෆⅆᒣᒾ㢮ࡢ $V&H ẚᑐ $V ྵ᭷㔞࠾ࡼࡧ㸪
6E&H ẚᑐ 6E ྵ᭷㔞㸬ẚ㍑ࡢࡓࡵ࡟༓ᓥᘼ㸪࢝ࢫࢣ࣮ࢻᘼࡢ⋞Ṋᒾࡢ⤌ᡂ⠊ᅖ㸦1ROOHWDO㸧ࢆ♧ࡋࡓ

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 ᅗ  ࡟♧ࡋࡓࡼ࠺࡟㸪$V&H ẚ㸪6E&H ẚࡣᗈ⠊ᅖ࡟ࡤࡽࡘࡁ㸪ሁ✚≀ࡢ࣐ࢢ࣐ࢯ࣮ࢫ࡬ࡢᐤ୚ࢆ♧၀ࡍࡿࢺࣞࣥࢻࢆᙧᡂࡍࡿ㸬 $V&H ẚ㸪6E&H ẚ࡟ࡘ࠸࡚ࡶヨᩱࡢᆅᇦ࡟ࡼࡿศ
ᩓࡀ኱ࡁࡃ㸪ᮾすኚ໬ഴྥࡣぢࡽࢀ࡞࠿ࡗࡓ㸬ࡓࡔࡋ㸪ྠᆅᇦ࡛ぢࡿ࡜㸪$V&H ẚ㸪6E&H ẚ࡜ࡶ㸪⋞Ṋᒾࡼࡾࡣ㧗 0J Ᏻᒣᒾࡢ᪉ࡀ㧗࠿ࡗࡓ㸦⾲㸯㸧㸬୍⯡࡟ࡇࢀࡲ࡛ከࡃࡢᚤ㔞ඖ⣲㸪ྠ఩య⤌ᡂ࡟ᇶ࡙ࡃ㆟ㄽ࠿ࡽࡣ㸪㧗 0J Ᏻᒣᒾ࡟ࡘ࠸࡚㸪ࡼࡾ㸪ࢫࣛࣈ⏤᮶ᡂศࡢῧຍࡢᗘྜ࠸ࡀ኱ࡁ࠸࡜ุ᩿ࡉࢀࡿࡇ࡜࡜ᩚ
ྜⓗ࡛࠶ࡿ㸬
 6KRGRVKLPD  $V
6E61. EDVDOW   
61. +0$  
2VDND $V6E6% EDVDOW  
1% +0$  
⾲㸯㸸ᑠ㇋ᓥ࠾ࡼࡧ኱㜰ᆅᇦࡢ㸪⋞Ṋᒾ࠾ࡼࡧ㧗 0JᏳᒣᒾࡢࣄ⣲㸪࢔ࣥࢳࣔࣥྵ᭷㔞 SSP ࡲࡓ㸪඲⯡࡟༓ᓥᘼ㸪࢝ࢫࢣ࣮ࢻᘼࡢ⋞Ṋᒾ࡜ẚ㍑
ࡋ࡚㸪$V&H ẚ㸪6E&H ẚࡶ㸪ࣄ⣲㸪࢔ࣥࢳࣔࣥࡢྵ
᭷㔞⮬యࡶ㧗࠸ヨᩱࡀከ࠸㸬 ࡲࡓࠊᅗ  ࡟ࡣ㸪ỿࡳ㎸ࡴሁ✚≀ࡢ⤌ᡂࢆ᪥ᮏࡢ
௜ຍయሁ✚≀㸦7RJDVKLHWDO㸧ࡸ༡ᾏࢺࣛࣇ ࡢ 㝣※ ሁ✚ ≀ ࠾ࡼ ࡧᅄ ᅜ ᾏ┅ ࡢ㐲 ὒ ᛶሁ ✚≀㸦6KLPRGDHWDO㸧ࡢࢹ࣮ࢱ࡟ᇶ࡙࠸࡚᥎ᐃ
ࡋࡓࡶࡢࡶ♧ࡋࡓ㸬୍㒊ࡢヨᩱࡣ㸪ሁ✚≀⮬యࡼࡾ$V&H ẚ㸪6E&H ẚࡀ㧗ࡃࠊ࣐ࢢ࣐ࢯ࣮ࢫ࡬ࡢῧຍࡣ㸪࣓ࣝࢺࡲࡓࡣὶయࢆ፹య࡟ࡋ࡚࠸ࡿࡇ࡜ࢆ᫂☜࡟♧ࡋ࡚࠸ࡿ㸬
㸦㸲㸧௒ᚋࡢ◊✲᪉㔪  ᖺᗘࡼࡾࠕ୰ᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡿⅆᡂᒾሁ✚ᒾ୰ࡢぶ㖡ඖ⣲ࡢᐃ㔞ࠖ࡜࠸࠺ㄢ㢟࡛㸪ࣄ⣲㸪࢔ࣥࢳࣔࣥ➼ࡢศᯒࢆࡉࡽ࡟⥅⥆ࡋ࡚ヨࡳࡼ࠺࡜ࡋ
࡚࠸ࡿ㸬ࡑࡢ୰࡛ࡣ㸪௨ୗࡢ㸰Ⅼ࡟ࡘ࠸࡚␃ពࡋ࡚
◊✲ࢆ㐍ࡵࡓ࠸㸬D ᶆ‽ヨᩱࡢ㑅ᐃ㸸ࡇࢀࡲ࡛㸪ᮍ▱ヨᩱ࡜ྠ᫬࡟㸪ᵝࠎ࡞ᶆ‽ヨᩱࢆ↷ᑕࡋศᯒࢆ⾜࡞ࡗࡓ㸬ඛ࡟グࡋࡓࡼ࠺࡟㸪௒ᅇࡣ⏘ᴗᢏ⾡⥲ྜ◊✲ᡤ㸪ᆅ㉁ㄪ
ᰝ⥲ྜࢭࣥࢱ࣮ࡢᆅ⌫໬Ꮫᶆ‽ヨᩱ -$㸦Ᏻᒣ

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ᒾ㸧ࢆᶆ‽࡜ࡋ࡚ᑐẚἲ࡛⾜ࡗࡓศᯒ⤖ᯝࢆሗ࿌ࡋࡓ㸬ࡑࢀ௨እ࡟㸪ྠࡌࡃ⏘ᴗᢏ⾡⥲ྜ◊✲ᡤࡢᆅ⌫໬Ꮫᶆ‽ヨᩱࡢ -5㸦ὶ⣠ᒾ㸧ࡸ
&50D㸦ᾏᗏ㉁㸸⏘ᴗᢏ⾡⥲ྜ◊✲ᡤ㸪ィ㔞ᶆ‽⥲ྜࢭࣥࢱ࣮ࡢ⎔ቃศᯒ⏝⤌ᡂᶆ‽≀㉁㸧㸪
650E㸦&RDOIO\DVK1,67 ᶆ‽ヨᩱ㸧ࡶేࡏ࡚↷ᑕ㸪ศᯒࢆ⾜ࡗࡓ㸬࠸ࡃࡘ࠿ࡢ ᐃᅇ࡟࠾࠸࡚㸪-$ ࢆᶆ‽࡜ࡋ࡚ồࡵࡓศᯒ್࡜㸪
650E ࢆᶆ‽࡜ࡋ࡚ồࡵࡓศᯒ್ࢆẚ㍑ࡋ
ࡓሙྜ㸪≉࡟ࣄ⣲࡟ࡘ࠸࡚᭱኱ 㸣⛬ᗘࡢᕪ␗ࡀぢࡽࢀࡓ㸬௒ࡢ࡜ࡇࢁࡑࡢཎᅉࡣ୙࡛᫂࠶ࡾ㸪௒ᚋࡶ」ᩘࡢᶆ‽ヨᩱࢆ↷ᑕࡋࢡࣟࢫ࡛ศᯒ್ࢆ᳨ウࡋ㸪㐺ษ࡞ᶆ‽ヨᩱࡢ㑅ูࢆ⾜࠺ᚲせࡀ࠶ࡿ㸬E ࡼࡾᗈ࠸✀㢮ࡢศᯒヨᩱ࡬ࡢ㐺⏝㸸ࡇࢀࡲ࡛グ
ࡋࡓ㏻ࡾ㸪⌧ᅾࡲ࡛ࡣ℩ᡞෆⅆᒣᒾ㢮㸪≉࡟㧗
0JᏳᒣᒾ࠾ࡼࡧ⋞Ṋᒾࢆ୰ᚰ࡟ศᯒࢆ⾜࡞ࡗ࡚ࡁࡓ㸬ᑗ᮶ⓗ࡟ࡣ㸪ࡼࡾᗈ࠸ヨᩱ✀࡟ࡘ࠸࡚ศᯒࢆ㐍ࡵࡓ࠸㸬ⅆᒣᒾヨᩱ࡜ࡋ࡚ࡣ㸪す༡᪥ᮏࡢ୰᪂ୡⅆᒣᒾ࡜ྠᵝ࡟㸪㧗 ࡢࢫࣛࣈỿࡳ
㎸ࡳࡀぢࡽࢀࡿᆅᇦࡢᓥᘼⅆᒣᒾ࡟ຍ࠼࡚㸪ẚ
㍑ⓗప ࡢࢫࣛࣈࡀỿࡳ㎸ࡴᆅᇦࡢᓥᘼⅆᒣᒾ࡟ࡘ࠸࡚㐺ᛂࡍࡿࡇ࡜ࢆィ⏬ࡋ࡚࠸ࡿ㸬ࡲࡓ㸪ࡇࢀࡽᓥᘼࡢⅆᒣᒾ࡟࠾ࡅࡿࢫࣛࣈ⏤᮶ᡂศ࡜ࡋ࡚㔜せ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡿ㸪ሁ✚ᒾ㢮࡟ࡘ࠸࡚ࡶ㐺ษ࡞ヨᩱࢆ཰㞟ࡋศᯒࢆ⾜࠸ࡓ࠸࡜⪃࠼࡚࠸ࡿ㸬≉࡟㸪௒ᅇሗ࿌ࡋࡓ℩ᡞෆⅆᒣᒾ㢮ࡢ࣐ࢢ࣐ࢯ࣮ࢫ࡟㛵㐃ࡍࡿࡶࡢ࡜ࡋ࡚ࡣ㸪す༡᪥ᮏࡢ௜ຍయሁ✚≀࡞࡝ࡀ㔜せ࡞ᑐ㇟≀࡛࠶ࡿ࡜⪃࠼࡚࠸ࡿ㸬ࡉࡽ࡟㸪ࣄ⣲ࡸ㸪࢔ࣥࢳࣔࣥࡣὶయ࡟ࡼࡿ⛣ືࠊ≉࡟ⅆᒣᘼࡼࡾὸᡤࡢࠊ
㧗ᅽᆺኚᡂస⏝ࡢ㡿ᇦ࡛ࡢ⛣ືࡶ▱ࡽࢀ㸪ኚᡂᒾᒾ▼Ꮫࡢ❧ሙ࠿ࡽ㆟ㄽࡉࢀ࡚࠸ࡿ㸦ࡓ࡜࠼ࡤ%HERXW㸧㸬ࡑࡇ࡛㸪୕Ἴᕝኚᡂᒾ࡞࡝ࡢ
㧗ᅽኚᡂᖏࡢሁ✚ᒾ⏤᮶ࡢ⤖ᬗ∦ᒾࡶศᯒᑐ
㇟࡜ࡋ࡚㸪᳨ウࡋ࡚ࡺࡁࡓ࠸㸬㸦㸳㸧ᡂᯝࡢබ⾲
࠙Ꮫ఍Ⓨ⾲ࠚ
᪂ṇ⿱ᑦ࣭ᢡᶫ⿱஧࣭ゅ஭ᮅ᫛࣭⚟ᒸᏕ᫛࣭
㛗㇂୰฼᫛࣭బ㔝㈗ྖ  ℩ᡞෆⅆᒣᒾ㢮ࡢ࣍࢘⣲ྵ᭷㔞᪥ᮏᆅ⌫ᝨᫍ⛉Ꮫ㐃ྜ  ᖺ኱఍㸦ᖥᙇ࣓ࢵࢭ㸧

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3-8Ἑᕝ࣭ỶỈᇦ࠾ࡼࡧᾏὒᗏሁ✚≀ࡢᨺᑕ໬ศᯒ
Activation analysis of river, estuarine and marine sedimentsᯇᑿᇶஅ࣭ஂ㔝❶ோ࣭ᑠ㇋ᕝ຾ぢ࣭㛗㇂ᕝ⠜ 1࣭ㅖ⏫኱ᆅ㧗ᶫ㯞Ꮚ࣭ᒣࣀ஭ಇ 2࣭ᫍ㔝┿᭷⨾ 3࣭ᒣ㔝Ꮥᕊ 3࣭ཎ┤ᶞ࣭⸨஭ᨻග 3ᮾி኱Ꮫ኱Ꮫ㝔⥲ྜᩥ໬◊✲⛉ᗈᇦ⛉Ꮫᑓᨷ
1 ᮾிᾏὒ኱Ꮫ኱Ꮫ㝔ᾏὒ⛉Ꮫᢏ⾡◊✲⛉ᾏὒಖ඲Ꮫᑓᨷ
2 ᮾி኱Ꮫ኱Ꮫ㝔⌮Ꮫ⣔◊✲⛉໬Ꮫᑓᨷ
3 ᮾி኱Ꮫᩍ㣴Ꮫ㒊ᗈᇦ⛉Ꮫ⛉㸯㸬ࡣࡌࡵ࡟

ᐖࢆッ࠼࡚࠸ࡿࡀࠊ⚟ᒸ㧗⿢ࡣ⛉Ꮫⓗ࡞ド᫂ࡀ࡞㏆ᖺࠊἙཱྀᇦࡸᖸ₲ࡢ⎔ቃಖ඲ࡣேࠎࡢ㔜኱࡞࠸࡜ࡋ࡚ッ࠼ࢆ㏥ࡅࠊబ㈡ᆅ⿢ࡣỈ㛛ᖖ᫬㛤ᨺ࡜㛵ᚰ஦࡜࡞ࡗ࡚࠸ࡿࡀࠊࡇࢀࡽࡢሙᡤࡣࠊῐỈ࡜ㄪᰝࢆᅜ࡟࿨ࡌ࡚࠸ࡿࠋࡇࡢࡼ࠺࡟ࠊᖸᣅࡸᇙ❧ᾏỈࡀΰࡊࡾྜ࠺」㞧࡞⣔࡛࠶ࡾࠊࡑࡇ࡟࠾ࡅࡿ

࡚ࡀ࿘㎶࡟ཬࡰࡍᙳ㡪ࡣᮍゎ࡛᫂࠶ࡾࠊࡇࢀࡽࢆ

໬Ꮫⓗ⎔ቃࡸඖ⣲ࡢᣲື࡟ࡘ࠸࡚ࡣࠊࡲࡔヲࡋࡃ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࡀ♫఍ⓗ࡟ࡶ⛉Ꮫⓗ࡟ࡶồࡵࡣ⌮ゎࡉࢀ࡚࠸࡞࠸ࠋᨺᑕ໬ศᯒἲࡣࠊከඖ⣲ྠࡽࢀ࡚࠸ࡿࠋᮏ◊✲࡛ࡣࠊᇙ❧࡚ࡢᙳ㡪ࡀᴟ➃࡟᫬ᐃ㔞ศᯒࡀྍ⬟࡞ࡓࡵࠊከࡃࡢඖ⣲ࡢศᕸࢆ⥲኱ࡁ࠿ࡗࡓ࡜⪃࠼ࡽࢀࡿ༓ⴥ┴㇂ὠᖸ₲࡜ࠊࡑࡢྜⓗ࡟ุ᩿ࡍࡿࡢ࡟᭱㐺࡞ศᯒἲ࡜ゝ࠼ࡿࠋᡃࠎ

ࡍࡄࡑࡤ࡟࠶ࡾ࡞ࡀࡽẚ㍑ⓗᙳ㡪ࡀᑠࡉ࠸࡜⪃ࡣࡇࢀࡲ࡛ 57Fe ࣓ࢫࣂ࢘࢔࣮ศගἲࢆ⏝࠸ࠊ㕲ࡢ࠼ࡽࢀࡿ୕␒℩⊧ᐇᕝἙཱྀ௜㏆ࢆᑐ㇟࡜ࡋ࡚ࠊᙜ

໬Ꮫ≧ែࢆᣦᶆ࡜ࡋ࡚Ἑᕝᗏ㉁ࡢ໬Ꮫⓗ⎔ቃࠊ≉◊✲ᐊ࡛Ἑཱྀᇦᗏ㉁ࡸᖸ₲ᗏ㉁࡟⏝࠸ࡽࢀ࡚ࡁ

࡟㓟໬㑏ඖ≧ែࢆ᥎ᐃࡋ࡚ࡁࡓࠋࡇࢀ࡟ᑐࡋࠊᚑ

ࡓศᯒᡭἲ࠾ࡼࡧ⤫ィⓗᡭἲࢆ⏝࠸࡚ࠊᇙ❧࡚ࡀ᮶ከࡃࡢ◊✲࡟ࡼࡾࠊヨᩱ୰ࡢᚤ㔞ඖ⣲ࡢศᕸࡀ࿘㎶࡟୚࠼ࡓᙳ㡪ࢆㄪᰝࡋࡓࠋࡲࡓࠊᖸ₲ᗏ㉁୰

໬Ꮫⓗ⎔ቃࢆ཯ᫎࡍࡿࡇ࡜ࡶ▱ࡽࢀ࡚࠸ࡿࠋᮏ◊࡛ࡣ◲㓟㑏ඖ⳦ࡢάື࡟ࡼࡾ◲໬Ỉ⣲ࡀⓎ⏕ࡋࠊ✲࡛ࡣࠊ࣓ࢫࣂ࢘࢔࣮ศගἲ࡟ࡼࡾᚓࡽࢀࡓ㕲ࡢ

ᗏ㉁୰ࡢ㕲࢖࢜ࣥ࡜཯ᛂࡋ◲໬㕲ࡸ pyrite(FeS2)

໬Ꮫ≧ែ࡜ࠊฟ᮶ࡿࡔࡅከࡃࡢᚤ㔞ඖ⣲ࡢศᕸ࡜ࢆ⏕ᡂࡍࡿࡇ࡜࠿ࡽࠊ࣓ࢫࣂ࢘࢔࣮ศගἲ࡟ࡼࡾ

ࡢ㛵㐃ࢆㄪ࡭ࠊẚ㍑᳨ウࡍࡿࡓࡵ࡟ከඖ⣲ྠ᫬ศ㕲ࡢ໬Ꮫ≧ែࢆ

ᯒࡀྍ⬟࡞ᨺᑕ໬ศᯒࢆ⾜ࡗࡓࠋࡇࡢࡼ࠺࡞ほⅬ࠙ᐇ㦂ࠚ㇂ὠᖸ₲ࡣࠊඖࡣᮾி‴ዟ࡟ᗈࡀࡿᗈ኱

࠿ࡽࠊḟ࡟ᥖࡆࡿヨᩱ࡟ࡘ࠸࡚✀ࠎࡢ⎔ቃ໬Ꮫⓗࠊ࡞๓὾ᖸ₲ࡢ୍㒊࡛࠶ࡗࡓࡀࠊᇙ❧࡚࡟ࡼࡾᅄ᪉

ᆅ⌫໬Ꮫⓗ࡞᳨ウࢆ⾜ࡗࡓࡢ࡛ࠊࡑࢀࡒࢀࡢヨᩱࡀ㝣ᆅ࡜࡞ࡗࡓ㛗᪉ᙧࡢᖸ₲࡛ࠊᮾி‴࡜ࡣ㸰ᮏࡈ࡜࡟◊✲ෆᐜ࠾ࡼࡧࡑࡢ⤖ᯝࢆሗ࿌ࡍࡿࠋ

ࡢ⣽࠸Ỉ㊰࡟ࡼࡗ࡚ࡘ࡞ࡀࡗ࡚࠸ࡿࠋᇙ❧࡚ᚋࠊᐃࡋࡓࠋࡉࡽ࡟㧗ᯫᶫ࡟ࡼࡗ࡚኱ᑠ㸰ࡘࡢ࢚ࣜ࢔࡟ศ᩿
㸰㸬ᖸ₲ᗏ㉁ࡢඖ⣲ศᕸ࡟ཬࡰࡍ࿘㎶㒊ᇙ❧࡚ࡢࡉࢀࡓࡇ࡜࠿ࡽࠊࡑࢀࡒࢀࡢ࢚ࣜ࢔࡛ᗏ㉁ヨᩱࢆᙳ㡪࡟㛵ࡍࡿ◊✲ᰕ≧࡟⣙  ੉᥇ྲྀࡋࡓࠋᚓࡽࢀࡓヨᩱࢆ㸱੉ࡈ࠙ᗎࠚ⎔ቃព㆑ࡀ㧗ࡲࡾࠊᖸ₲ࡢᇙ❧࡚୰Ṇࡸಖ࡜࡟ษࡾศࡅࠊ✵Ẽ࡟ࡼࡿ㓟໬࡟ὀពࡋ࡞ࡀࡽࠊ

඲࣭෌⏕ࡢືࡁࡀάⓎ໬ࡋ࡚࠸ࡿࠋ୍᪉࡛ࠊㅋ᪩

❅⣲ຍᅽℐ㐣࡟ࡼࡾ㛫㝽Ỉ࡜‵ヨᩱ࡟ศ㞳ࡋࠊ‵‴ᖸᣅ஦ᴗࡀ᩿⾜ࡉࢀࠊ᭷᫂ᾏࡢ⁺Ẹࡽࡀ⁺ᴗ⿕

ヨᩱࡢ୍㒊ࢆ෾⤖஝⇱࡟ࡼࡾ஝⇱ヨᩱ࡜ࡋࡓࠋࡇ◊✲᪋タ࡜⿦⨨ྡ                ◊✲ศ㔝
 JRR-4ࠊJRR-3MࠊẼ㏦⟶ࠊȚ⥺㺛㺫㺽㺖㺢㺹㺰㺎㺞㺎     ⎔ቃ໬Ꮫࠊᆅ⌫໬Ꮫࠊᨺᑕ໬ศᯒ

- 343 -

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JAEA-Review 2013-039

ࢀࡽࡢ᧯సࡢ๓ᚋࡢ㔜㔞ኚ໬࠿ࡽྵỈ⋡ࢆồࡵࠊࣥࢱࣛࢡࢩࣙࣥࡀᙉࡲࡾࠊ⁐Ꮡ㓟⣲㔞ࡀቑຍࡋ‵ヨᩱࢆ⏝࠸࡚࣓ࢫࣂ࢘࢔࣮ศගἲ࡟ࡼࡾ Fe ࡢ࡚㑏ඖᗘྜࡀᙅࡲࡗࡓࡶࡢ࡜⪃࠼ࡽࢀࡿࠋ

≧ែศᯒࢆ⾜࠸ࠊ஝⇱ヨᩱࢆ⏝࠸࡚ᶵჾ୰ᛶᏊᨺ
(PGA)࡟ࡼࡾඖ⣲ࡢᆶ┤ศᕸࢆồࡵࡓࠋ࠙⤖ᯝཬࡧ⪃ᐹࠚ㇂ὠᖸ₲୧ᆅⅬ࡟࠾࠸࡚࿘㎶ᇙ❧࡚ࡢᙳ㡪࡜⪃࠼ࡽࢀࡿ኱ࡁ࡞ኚ໬ࡀྛ

ᐃࡢ⤖ᯝ࡟⌧ࢀ࡚࠸ࡓࠋ୍᪉ࠊ୕␒℩ヨᩱ࡟ࡘ࠸࡚ࡣ

6➨୍୺ᡂศᚓⅬ

ᑕ໬ศᯒ(INAA)࠾ࡼࡧ୰ᛶᏊㄏ㉳༶ⓎȚ⥺ศᯒ

0
Ͳ3
Ͳ6

㇂ὠᖸ₲ࡢࡼ࠺࡞┠❧ࡗࡓኚ໬ࡣぢࡽࢀ࡞࠿ࡗ
ࡓࠋᚓࡽࢀࡓ

30ᐃ⤖ᯝࡢ࠺ࡕࠊINAA ࡜ PGA ࡟ࡼࡿඖ⣲ᆶ┤ศᕸࡢࢹ࣮ࢱ࡟ᑐࡋ࡚୺ᡂศศᯒ
࠸ࡿ᪉ἲ࡜┦㛵⾜ิࢆ⏝࠸ࡿ᪉ἲࡢ஧ᡭἲࡀᏑ
ᅾࡍࡿࠋ๓⪅ࡣࢹ࣮ࢱࡢ್ࢆࡑࡢࡲࡲ཯ᫎࡉࡏࡿ
ࡢ࡟ᑐࡋࠊᚋ⪅ࡣࢹ࣮ࢱࢆศᩓ 㸪ᖹᆒ  ࡟ᶆ‽໬ࡋࡓ್ࢆ⏝࠸ࡿࠋᮏ◊✲࡛ࡣࡲࡎࠊ୧ᡭἲࡢẚ0⤖ᯝࢆ♧ࡍࠋࡇࡢᆅⅬ࡛ࡣࠊ࿘㎶ᇙ❧࡚ࡢᙳ㡪ࡀ

୺ᡂศᚓⅬࡶᇙ❧࡚ࡸศ᩿ࡢᙳ㡪ࢆ཯ᫎࡋ࡚࠸
ࡿ࡜ᛮࢃࢀࡿ್ࢆ♧ࡋࠊᅛ᭷࣋ࢡࢺࣝࡢ್ࡀᖹᆒ
⃰ᗘ࡜┦㛵ࡏࡎ࡟ᚤ㔞ඖ⣲ࡀ୺せඖ⣲࡜ྠᵝ࡟

4

6

Ͳ2
Ͳ4
Ͳ6

log|ᖹᆒ⃰ᗘ/ppm|⣙  ੉㸪ศ᩿ࡢᙳ㡪ࡀ  ੉ࡢ῝ࡉ࡟⌧ࢀ࡚࠸ࡓࠋ
ᮏᡭἲࢆ⏝࠸ࡓሙྜࡢࡳࠊ➨୍୺ᡂศᚓⅬࡶ➨஧

2

depth/cm

0log|ᅛ᭷䝧䜽䝖䝹|ࡿヨᩱ࡟ᑐࡍࡿୖグ㸱ᡭἲ࡟ࡼࡿ୺ᡂศศᯒࡢ

60

Ͳ2

0

࡜➨㸰୺ᡂศ௨㝆ࡀࣀ࢖ࢬ࡜ࡋ࡚ࡋ࠿ゎ㔘࡛ࡁ⾜ࡗࡓࠋᅗ㸯࡟ࠊ㇂ὠᖸ₲ࡢᑠࡉ࠸࢚ࣜ࢔࡟࠾ࡅ

400⪃៖ࡉࢀ࡞࠸⤖ᯝ࡜࡞ࡗࡓࠋ୍᪉ࠊᚋ⪅ࢆ⏝࠸ࡿࡋࡓୖ࡛ศᩓඹศᩓ⾜ิࢆ⏝࠸࡚୺ᡂศศᯒࢆ

20

2ࡢ኱ࡁࡉࡀᙳ㡪ࡋࠊᚤ㔞ඖ⣲ࡢࢹ࣮ࢱࡀ࡯࡜ࢇ࡝

ࢱࢆྛඖ⣲ࡢᖹᆒ⃰ᗘ࡛๭ࡾࠊᖹᆒࢆ㸯࡟つ᱁໬60

Ͳ4㍑ࢆ⾜ࡗࡓࠋࡑࡢ⤖ᯝࠊ๓⪅ࢆ⏝࠸ࡿ࡜ࡤࡽࡘࡁ

࡞࠸⤖ᯝ࡜࡞ࡗࡓࠋࡑࡇ࡛ࠊඖ⣲ᆶ┤ศᕸࡢࢹ࣮

40

4➨஧୺ᡂศᚓⅬࢆ⾜ࡗࡓࠋ୺ᡂศศᯒ࡛ࡣࠊศᩓඹศᩓ⾜ิࢆ⏝

20

depth/cm

ศᩓඹศᩓ⾜ิ䜢⏝䛔䛯୺ᡂศศᯒ
┦㛵⾜ิ䜢⏝䛔䛯୺ᡂศศᯒ
ᮏᡭἲᢅࢃࢀ࡚࠸ࡿࡇ࡜ࡀࢃ࠿ࡗࡓࠋ

ᅗ㸯㸬㸱ᡭἲ࡟ࡼࡿ୺ᡂศศᯒࡢ⤖ᯝẚ㍑

 ḟ ࡟ ࠊ ࣓ࢫ ࣂ ࢘ ࢔ ࣮ศ ග ἲ ࡟ ࡼࡾ ᚓ ࡽ ࢀ ࡓୖẁ㸸➨୍୺ᡂศᚓⅬ  ୰ẁ㸸➨஧୺ᡂศᚓⅬ

pyrite(FeS2)ࡢᆶ┤ศᕸࢆᅗ㸰࡟♧ࡍࠋࡇࢀࡽࡢ

ୗẁ㸸ྛඖ⣲ࡢ➨୍୺ᡂศࡢᅛ᭷࣋ࢡࢺࣝ࡜ᖹᆒ⃰ᗘࡢ㛵ಀ⤖ᯝ࡜ྵỈ⋡ࡸ᭷ᶵ≀㔞࡞࡝௚ࡢᐃ⤖ᯝ࡜ࡢẚ㍑࠿ࡽࠊ➨୍୺ᡂศࡣሁ✚᫬ࡢỈࡢὶࢀࡢᙅࡉ

40ࢆ♧ࡍᣦᶆࠊ➨஧୺ᡂศࡣሁ✚ᚋࡢᾏỈ࡜ࡢ࢖ࣥ30ࢱࣛࢡࢩࣙࣥࡢᙉࡉࢆ࠶ࡽࢃࡍᣦᶆ࡜࡞ࡿ࡜⪃20࠼ࡽࢀࡿࠋࡍ࡞ࢃࡕࠊᇙ❧࡚࡟ࡼࡾᾏỈࡢὶࢀ

10ࡀᙅࡲࡾ㑏ඖⓗ⎔ቃ࡜࡞ࡗࡓᚋࠊ㧗ᯫᶫ࡟ࡼࡿ

0ศ᩿࡟ࡼࡾ⊃࠸Ỉ㊰ࡢࡼ࠺࡞≧ែ࡟࡞ࡗࡓࡓ
ࡵࠊ༢఩㠃✚࠶ࡓࡾࡢὶ㔞ࡀቑ࠼ࠊᾏỈ࡜ࡢ࢖- 344 -

Pyrite(%)

0

20

40

ᅗ㸰㸬 ㇂ὠᖸ₲ᗏ㉁ࡢ pyrite ࡢᆶ┤ศᕸ

3-8
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JAEA-Review 2013-039

㸱㸬ᮾி‴ឤ₻ᇦᗏ㉁࡟࠾ࡅࡿ㓟໬㑏ඖ㟁఩࡜ඖ࡜࡛ࠊpyrite(FeS2)ࡀ⏕ᡂࡍࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸⣲ࡢᣲືࡿࠋࡼࡗ࡚ᮏ◊✲࡟࠾࠸࡚ Fe ࡜ S ࡢ࣮ࣘࢡࣜࢵ

࠙ᗎࠚᮾி‴࡛ࡣ㏆ᖺỈ㉁ࡀᨵၿࡋࡓ࡜ゝࢃࢀ࡚ࢻ㊥㞳ࡀ㏆࠸ࠊࡘࡲࡾᗏ㉁୰࡛ࡢᣲືࡀఝ㏻ࡗ࡚

࠸ࡿࡀࠊ㟷₻ࡢⓎ⏕࡟ࡼࡾ⁺ᴗ࡬ࡢᙳ㡪ࡀሗ࿌ࡉ࠸ࡓ࡜࠸࠺ࡇ࡜ࡣࠊ◲㓟㑏ඖࡢᙳ㡪ࢆホ౯ࡍࡿୖࢀࡿ➼ࠊ௒᪥࡛ࡶᮍゎỴࡢၥ㢟ࢆᢪ࠼࡚࠸ࡿࠋ

࡛ព⩏ࡀ࠶ࡿ⤖ᯝࡔ࡜⪃࠼ࡽࢀࡿࠋࡲࡓࠊ㑏ඖⓗ2008 ᖺ 7 ᭶࡟ࡣ⎔ቃ┬ࡸྛἢᓊ⮬἞య(46 ᶵ㛵࣭⎔ቃୗ࡛ࡣ⁐ฟࡍࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ Mn ࡣࠊᅋయ)࡟ࡼࡿỈ㉁⎔ቃㄪᰝࡀᮾி‴ෆ 568 ࢝ᡤ࡛

῝ᒙࡢヨᩱ࡛ࡣ⾲ᒙࡢヨᩱ࡟ẚ࡭ῶᑡࡀぢࡽࢀࠊ⾜ࢃࢀࠊኟᮇ࡟࠾ࡅࡿᮾி‴ࡢ㖄┤᪉ྥࡢ⁐Ꮡ㓟௚ࡢඖ⣲࡜ࡢ࣮ࣘࢡࣜࢵࢻ㊥㞳ࡀ኱ࡁࡃ࡞ࡗ࡚

⣲㔞ࡢศᕸࡸ㈋㓟⣲Ỉሢࡢᐇែࢆ᫂ࡽ࠿࡟ࡋ࡚

࠸ࡓࠋࡇࢀࡽ࠿ࡽࠊᗏ㉁୰ࡢඖ⣲⃰ᗘࡢ㖄┤ศᕸ࠸ࡿࠋࡋ࠿ࡋࠊࡇࡢㄪᰝ࡛ࡣ⁐Ꮡ㓟⣲㔞࣭Ỉ࣭

ࡀࠊORP ኚ໬࡟ࡼࡗ࡚኱ࡁ࡞ᙳ㡪ࢆཷࡅ࡚࠸ࡿࡇ

ሷศ⃰ᗘ࡞࡝ࡢỈ㉁⎔ቃ࡟㛵ࡍࡿㄪᰝ⤖ᯝࡢࡳ࡜ࡀ♧၀ࡉࢀࡓࠋࡲࡓࠊCr ࡸ Zn ➼ࡢேⅭ㉳※ࡀ

ࡀሗ࿌ࡉࢀ࡚࠸ࡿ⌧≧࡛࠶ࡾࠊᗏ㉁࡟㛵ࡍࡿࢹ࣮␲ࢃࢀࡿඖ⣲࡟ࡘ࠸࡚ࡣࠊ≉ᐃࡢ῝ࡉࡢヨᩱ࡛㢧ࢱࡣ୙༑ศ࡛࠶ࡿࠋ≉࡟Ἑཱྀᇦ(ឤ₻ᇦ)ࡣࠊ⏕≀ⴭ࡟ቑຍࡀぢࡽࢀࠊࡑࡢ௚ࡢඖ⣲࡜ࡢ᭷ពᕪࡀぢࡢ⏕⏘ᛶࡣ㧗࠸ࡀởᰁࡉࢀࡸࡍ࠸࡜࠸࠺≉ᚩࢆࡽࢀࡓࠋࡇࢀࡽࡢ⤖ᯝ࠿ࡽࠊከඖ⣲ࡢᐃ㔞್࡟ᑐᣢࡗ࡚࠾ࡾࠊ㏆ᖺ⎔ቃホ౯ࡢ㔜せᛶࡀ㧗ࡲࡗ࡚࠸ࡋࠊࢡࣛࢫࢱ࣮ศᯒࡸከḟඖᑻᗘᵓᡂἲ➼ࡢ⤫ィࡿࡀࠊ≀㉁཰ᨭ➼ࡢ࣓࢝ࢽࢬ࣒ࡣ㠀ᖖ࡟」㞧࡛࠶ⓗᡭἲࢆ㐺⏝ࡍࡿࡇ࡜࡛ࠊἙཱྀᇦᗏ㉁࡟ࡘ࠸࡚≉ࡾࠊせ⣲ẖࡢᙳ㡪ࢆホ౯ࡍࡿࡇ࡜ࡣᐜ࡛᫆ࡣ࡞࠸ࠋ ᚩⓗ࡞ඖ⣲ࡢᣲືࢆศ㢮࡛ࡁࡿࡇ࡜ࡀ♧၀ࡉࢀࡼࡗ࡚ᮏ◊✲࡛ࡣࠊᮾி‴ࡢὶධἙᕝ࡛࠶ࡿከᦶ

ࡓࠋᕝࡢἙཱྀᇦ࡟ࡘ࠸࡚ࠊᗏ㉁୰ࡢඖ⣲ࡢᐃ㔞್࡟⤫ィⓗฎ⌮ࢆ⏝࠸ࡿࡇ࡜࡛ࠊඖ⣲ࡢᣲືࡢ≉ᚩࢆぢฟࡍࡇ࡜ࢆ◊✲ࡢ┠ⓗ࡜ࡋࡓࠋ࠙ᐇ㦂ࠚἙཱྀᇦᗏ㉁ࡣࢥ࢔ࢧࣥࣉ࣮࡛ࣛ㖄┤᪉ྥ࡟᥇ྲྀࡋࡓࡶࡢࢆ῝ࡉ᪉ྥ࡟㸱੉ࡈ࡜࡟࢝ࢵࢺ
ࡋࠊຍᅽࢁ㐣ࢆ⾜ࡗࡓᚋࠊࣇ࣮ࣜࢬࢻࣛ࢖ࡋࡓࠋ
ᚓࡽࢀࡓ஝⇱ヨᩱ࡟ࡘ࠸࡚ࠊᶵჾ୰ᛶᏊᨺᑕ໬ศ
ᯒ࡜༶ⓎȚ⥺ศᯒࢆ⏝࠸࡚ከඖ⣲ࡢᐃ㔞ศᯒࢆ⾜ࡗࡓࠋᐃ㔞್ࡣࢹ࣮ࢱࡢ㢮ఝᗘࢆ࣮ࣘࢡࣜࢵࢻ
㊥㞳ࡢ኱ᑠ࡛⾲ࡍࢡࣛࢫࢱ࣮ศᯒ࡜ከḟඖᑻᗘᵓᡂἲ࡟ࡼࡿ⤫ィⓗᡭἲࢆ⏝࠸࡚ゎᯒࡋࠊ῝ᗘูࠊඖ⣲ู࡟ศ㢮ࢆ⾜࠸ࠊ㓟໬㑏ඖ㟁఩➼࡜ࡢ┦㛵࡟ᅗ㸱㸬ከᦶᕝἙཱྀᖸ₲ᗏ㉁ࡢ㓟໬㑏ඖ㟁఩ࡘ࠸࡚⪃ᐹࢆ⾜ࡗࡓࠋ࠙⤖ᯝ࡜⪃ᐹࠚᅗ㸱࡟ࠊከᦶᕝἙཱྀᖸ₲ᗏ㉁ࡢ㓟໬㑏ඖ㟁఩(ORP)ࡢ㖄┤ኚ໬ࢆ♧ࡍࠋ ੉௨῝ࡢヨᩱ࡛ࡣ ORP ࡣ㈇ࡢ್ࢆྲྀࡗ࡚࠸ࡓࠋࡇࡢ㓟໬㑏ඖ㟁఩ࡢṇ㈇ࢆࠊඖ⣲ศᯒ್ࡼࡾᚓࡽࢀࡓࢡࣛ
ࢫࢱ࣮ศᯒ➼ࡢ⤖ᯝ࡜⤌ࡳྜࢃࡏ࡚⪃࠼ࡿ࡜ࠊ
ORP ࡀṇࡢヨᩱ࡜㈇ࡢヨᩱ࡛ࠊ࣮ࣘࢡࣜࢵࢻ㊥㞳ࡀ኱ࡁࡃ࡞ࡿ࡜࠸࠺ഴྥࡀぢࡽࢀࡓ(ᅗ㸲)ࠋࡲࡓࠊ
ඖ⣲ูࡢẚ㍑࡛ࡣࠊORP ኚ໬࡟ࡼࡿᙳ㡪ࢆཷࡅࡸࡍ࠸࡜ゝࢃࢀࡿ Fe ࡜ S ࡢ࣮ࣘࢡࣜࢵࢻ㊥㞳ࡀ㏆࠸࡜࠸࠺ഴྥࡀぢࡽࢀࡓࠋἙᕝឤ₻ᇦ࡟࠾࠸࡚ࡣ
ᗏ㉁୰࡛㑏ඖⓗ⎔ቃࡀ⏕ࡌࠊ◲㓟㑏ඖࡀ㉳ࡇࡿࡇ- 345 -

ᅗ㸲㸬ከᦶᕝἙཱྀᖸ₲ᗏ㉁ࡢ῝ᗘูࢹࣥࢻࣟࢢ࣒ࣛ
(ORP ࡀ㈇ࡢヨᩱࢆ୸࡛ᅖࢇ࡛♧ࡋࡓ)

3-8
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JAEA-Review 2013-039

㸲㸬ᡂᯝࡢබ⾲Ꮫ఩ㄽᩥᏛ⾡ㄅࠊ⣖せ➼10. ᗏ㉁ࡢ໬Ꮫศᯒ࠿ࡽぢࡓᮾி‴࿘㎶ࡢぶỈ⎔

1. Estimation of the sources of pelagic sediments fromቃࡢホ౯ࠊᫍ㔝┿᭷⨾ࠊᮾி኱Ꮫᩍ㣴Ꮫ㒊ᗈᇦ

the South Pacific Ocean to the Antarctic Ocean, K.

⛉Ꮫ⛉ ༞ᴗㄽᩥϨ (2006 ᖺ 11 ᭶)

Shozugawa, A. Kuno, Y. Sano and M. Matsuo, J.

11. 㓟ᛶ㞵࡟ࡼࡿᅵተࡢ㓟୰࿴⬟ࡢ㖄┤ኚ໬ࠊ ᒣRadioanal. Nucl. Chem., Articles, 278, 331-335

㔝Ꮥᕊࠊᮾி኱Ꮫᩍ㣴Ꮫ㒊ᗈᇦ⛉Ꮫ⛉ ༞ᴗㄽᩥ(2008)

Ϩ (2006 ᖺ 11 ᭶)

2. Influence of reclamation on the concentrations and12. ከᦶᕝ࡜ࡑࡢᨭὶ࡟࠾ࡅࡿἙᕝ⎔ቃࡢホ౯

chemical states of elements in tideland sediment, D.

㹼ேⅭ㉳※≀㉁ࡢᙳ㡪ࢆ᥈ࡿ㹼ࠊཎ┤ᶞࠊᮾி

Moromachi, A. Kuno and M. Matsuo, J. Radioanal.

኱Ꮫᩍ㣴Ꮫ㒊ᗈᇦ⛉Ꮫ⛉ ༞ᴗㄽᩥϨ (2007 ᖺ

Nucl. Chem., Articles, 278, 495-498 (2008)11 ᭶)

3. Elemental analysis of airborne fine particles

13. 㞷ị୰ࡢ⢏Ꮚ≧≀㉁ࡢඖ⣲ศᯒ࡟ࡼࡿ኱Ẽởcollected at roadside of an arterial road, M.

ᰁ≀㉁ࡢᣲື࡟㛵ࡍࡿ◊✲ࠊ⸨஭ᨻගࠊᮾி኱

Hirabayashi, M. Matsuo, S. Hasegawa, S. KobayashiᏛᩍ㣴Ꮫ㒊ᗈᇦ⛉Ꮫ⛉ ༞ᴗㄽᩥϨ (2008 ᖺ 11

and K. Tanabe, J. Radioanal. Nucl. Chem., Articles,᭶)278, 479-483 (2008)14. ᖸ₲ᗏ㉁ࡢඖ⣲ศᕸ࡟ཬࡰࡍ࿘㎶㒊ᇙ❧࡚ࡢ

4. ༡ኴᖹὒ࡟࠾ࡅࡿ㐲ὒᛶሁ✚≀ࢆࣉ࣮ࣟࣈ࡜

ᙳ㡪࡟㛵ࡍࡿ◊✲ࠊㅖ⏫኱ᆅࠊᮾி኱Ꮫ኱Ꮫ㝔ࡋࡓሁ✚ᙜ᫬ࡢẼೃኚືࡢ᳨ウࠊᑠ㇋ᕝ຾ぢ࣭⥲ྜᩥ໬◊✲⛉ᗈᇦ⛉Ꮫᑓᨷ ಟኈㄽᩥ (2009㔠஭㇏࣭బ㔝᭷ྖ࣭ᯇᑿᇶஅࠊ
ࠕᨺᑕ໬ศᯒἲ฼

ᖺ 1 ᭶)⏝࡟㛵ࡍࡿᅜ㝿໬ࠖᑓ㛛◊✲఍ሗ࿌᭩ࠊி㒔኱15. 㓟ᛶ㞵⿕ᐖࡀぢࡽࢀࡿᆅᇦ࡟࠾ࡅࡿᅵተࡢඖ

ᏛཎᏊ⅔ᐇ㦂ᡤࠊ58-69 (2008)⣲ศᯒ࡜㓟୰࿴⬟࡜ࡢ㛵㐃ᛶࠊ㧗ᶫ㯞Ꮚࠊᮾி

5. Elemental analysis and acid neutralization capacity኱Ꮫ኱Ꮫ㝔⥲ྜᩥ໬◊✲⛉ᗈᇦ⛉Ꮫᑓᨷ ಟኈof soil at the area where the acid rain damage isㄽᩥ (2009 ᖺ 1 ᭶)observed, A. Takahashi, A. Kuno and M. Matsuo,

16. ஺᥮ᛶ㝧࢖࢜ࣥ࡟ࡼࡿᅵተࡢ㓟୰࿴⬟ࡢゎᯒࠊࠕᨺᑕ໬ศᯒἲ฼⏝࡟㛵ࡍࡿᅜ㝿໬ࠖᑓ㛛◊✲ᒣࣀ஭ಇࠊᮾி኱Ꮫ኱Ꮫ㝔⌮Ꮫ⣔◊✲⛉໬Ꮫᑓ఍ሗ࿌᭩ࠊி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤࠊ70-78 (2008)ᨷ ಟኈㄽᩥ (2009 ᖺ 2 ᭶)

6. ㇂ὠᖸ₲ཬࡧⰪᾆ㐠Ἑࡢᗏ㉁୰࡟࠾ࡅࡿỈ㉁17. ㇂ὠᖸ₲࠾ࡼࡧⰪᾆ㐠Ἑࡢᗏ㉁࣭㛫㝽Ỉ୰࡟ί໬స⏝ࡢゎᯒࠊ㛗㇂ᕝ⠜࣭⏣୰⨾✑࣭ஂ㔝❶࠾ࡅࡿί໬ᶵ⬟࡟㛵ࡍࡿ◊✲ࠊ㛗㇂ᕝ⠜ࠊᮾிோ࣭ᯇᑿᇶஅ, ศᯒ໬Ꮫ, 58, 87-94 (2009)ᾏὒ኱Ꮫ኱Ꮫ㝔ᾏὒ⛉Ꮫᢏ⾡◊✲⛉ᾏὒಖ඲Ꮫ

7. ㇂ὠᖸ₲ሁ✚≀୰ࡢί໬ᶵ⬟࡟࠾ࡅࡿ㛫㝽Ỉᑓᨷ ಟኈㄽᩥ (2009 ᖺ 3 ᭶)ࡢᙺ๭࡟㛵ࡍࡿ◊✲ࠊ㛗㇂ᕝ⠜࣭⏣୰⨾✑࣭㝰Ꮫ఍Ⓨ⾲಴ ┿࣭ஂ㔝❶ோ࣭ᯇᑿᇶஅ, ศᯒ໬Ꮫ, 58,

18. ᨺᑕ໬ศᯒἲࢆ⏝࠸ࡓ㐲ὒᛶᾏὒሁ✚≀⾲ᒙ

327-332 (2009)࡟࠾ࡅࡿ౪⤥※ࡢ᳨ウࠊᑠ㇋ᕝ຾ぢ࣭ஂ㔝❶ோ࣭

57

8. Fe Mössbauer study of specific iron species in theబ㔝᭷ྖ࣭ᯇᑿᇶஅࠊ➨ 51 ᅇᨺᑕ໬Ꮫウㄽ఍

Antarctic Ocean sediments, K. Shozugawa, A. Kuno,(2007 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍) (2007 ᖺ 9 ᭶)

H. Miura and M. Matsuo, J. Nucl. Radiochem. Sci.,

19. ᶵჾ୰ᛶᏊᨺᑕ໬ศᯒἲ㺃༶Ⓨ࣐࢞ࣥ⥺ศᯒ

10, 13-17 (2009)ἲ࡟ࡼࡿ⎔ቃヨᩱ㺃ᆅ⌫໬Ꮫⓗヨᩱࡢከඖ⣲ศ

9. ᮾி‴ឤ₻ᇦᗏ㉁࡟࠾ࡅࡿ㓟໬㑏ඖ㟁఩࡜ඖᯒࠊᯇᑿᇶஅ࣭ᑠ㇋ᕝ຾ぢ࣭ㅖ⏫኱ᆅࠊཎᏊຊ

⣲ࡢᣲື࡟㛵ࡍࡿ◊✲ࠊཎ┤ᶞ࣭ᑠ㇋ᕝ຾ぢ࣭ᶵᵓ᪋タ฼⏝୍⯡ඹྠ◊✲ᡂᯝሗ࿌఍ (2008 ᖺᯇᑿᇶஅࠊࠕி኱ཎᏊ⅔ࡢ෌㛤࡜ᨺᑕ໬ศᯒࠖᑓ

8 ᭶)㛛◊✲఍ሗ࿌᭩ࠊி㒔኱ᏛཎᏊ⅔ᐇ㦂ᡤࠊ53-59

20. ᖸ₲࠾ࡼࡧ㐠Ἑࡢᗏ㉁࣭㛫㝽Ỉ୰ࡢඖ⣲ศᯒ

(2009)

࡟ࡼࡿ⎔ቃホ౯ࠊ㛗㇂ᕝ⠜࣭⏣୰⨾✑࣭ᯇᑿᇶ3-8- 346 -

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JAEA-Review 2013-039

அࠊ᪥ᮏศᯒ໬Ꮫ఍➨ 57 ᖺ఍ (2008 ᖺ 9 ᭶)఍ᖺ఍) (2009 ᖺ 9 ᭶)

21. ᖸ₲ᗏ㉁୰ࡢඖ⣲ᆶ┤ศᕸ࡬ࡢ୺ᡂศศᯒࡢ

32. Neutron activation analysis of marine sediment㐺ᛂ࡟ࡼࡿ⎔ቃኚືࡢホ౯ἲࡢ᳨ウࠊㅖ⏫኱samples for environmental monitoring, M. Matsuo,ᆅ࣭ᯇᑿᇶஅࠊ᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ (2008 ᖺ 9

FNCA 2009 Workshop on Research Reactor

᭶)

Utilization, Hachinohe, (September 2009)22. ᅵተࡢ㓟୰࿴⬟࡬ᙳ㡪ࢆ୚࠼ࡿ஺᥮ᛶ Ca ࢖

3-8࢜ࣥࡢ໬Ꮫᙧែࠊᒣࣀ஭ಇ࣭ᑠ㇋ᕝ຾ぢ࣭ᯇᑿᇶஅࠊ᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ (2008 ᖺ 9 ᭶)
23. 㓟ᛶ㞵⿕ᐖࡀぢࡽࢀࡿᆅᇦ࡟࠾ࡅࡿᅵተࡢඖ
⣲ศᕸ࡜㓟୰࿴⬟࡜ࡢ㛵㐃ᛶࠊ㧗ᶫ㯞Ꮚ࣭ᑠ㇋ᕝ຾ぢ࣭ᯇᑿᇶஅࠊ᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ (2008ᖺ 9 ᭶)
24. ◲㓟㑏ඖ࡜ᰤ㣴ሷ࠿ࡽぢࡓ㒔ᕷἙᕝࡢ⎔ቃホ౯ࠊཎ┤ᶞ࣭ᑠ㇋ᕝ຾ぢ࣭ᯇᑿᇶஅࠊ᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ (2008 ᖺ 9 ᭶)
25. 㐣๫ 230Th ࡟ࡼࡾᖺ௦Ỵᐃࡉࢀࡓ㐲ὒᛶᾏὒሁ
✚≀⾲ᒙ࡟࠾ࡅࡿ Aragonite-Calcite ┦㌿⛣ࠊᑠ㇋ᕝ຾ぢ࣭㔠஭ ㇏࣭బ㔝᭷ྖ࣭ᯇᑿᇶஅࠊ➨ 52ᅇᨺᑕ໬Ꮫウㄽ఍ (2008 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍)(2008 ᖺ 9 ᭶)
26. ᨺᑕ໬ศᯒἲࢆ⏝࠸ࡓᖸ₲ࡢኚ㑄࡜ᗏ㉁୰ࡢ
ඖ⣲ᆶ┤ศᕸࡢ㛵㐃ᛶࡢ᳨ウࠊㅖ⏫኱ᆅ࣭ᯇᑿ
ᇶஅࠊ➨ 52 ᅇᨺᑕ໬Ꮫウㄽ఍ (2008 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍) (2008 ᖺ 9 ᭶)
27. 㓟୰࿴⬟ࡢほⅬ࠿ࡽぢࡓᅵተ࡟࠾ࡅࡿ Ca ࡢ྾╔ᙧែࡢศᯒࠊᒣࣀ஭ಇ࣭ᑠ㇋ᕝ຾ぢ࣭ᯇᑿᇶஅࠊ➨ 52 ᅇᨺᑕ໬Ꮫウㄽ఍ (2008 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍) (2008 ᖺ 9 ᭶)
28. ᗏ㉁࣭㛫㝽Ỉ୰ࡢ㕲ࡢᣲື࡟ࡼࡿᖸ₲ࡢί໬ᶵ⬟࡟㛵ࡍࡿ◊✲ࠊ㛗㇂ᕝ⠜࣭⏣୰⨾✑࣭ᯇᑿᇶஅࠊ➨㸳ᅇⲈᇛᆅ༊ศᯒᢏ⾡஺ὶ఍ (2008 ᖺ
10 ᭶)
29. Monitoring of environmental contamination andenvironmental changes, M. Matsuo, FNCA 2008
Workshop on Research Reactor Utilization, Vietnam,(October 2008)30. ᖸ₲ᗏ㉁࡟࠾ࡅࡿ㓟໬㑏ඖ㟁఩࡜ඖ⣲ࡢᣲື࡟㛵ࡍࡿ◊✲ࠊཎ┤ᶞ࣭ᑠ㇋ᕝ຾ぢ࣭ᯇᑿᇶஅࠊ
᪥ᮏᆅ⌫໬Ꮫ఍ᖺ఍ (2009 ᖺ 9 ᭶)
31. 㑏ඖⓗ⎔ቃୗ࡟࠾ࡅࡿᮾி‴ᗏ㉁࡟ྵࡲࢀࡿ
ඖ⣲ࡢ໬Ꮫ≧ែࠊཎ┤ᶞ࣭ᑠ㇋ᕝ຾ぢ࣭ᯇᑿᇶஅࠊ➨ 53 ᅇᨺᑕ໬Ꮫウㄽ఍ (2009 ᪥ᮏᨺᑕ໬Ꮫ

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3-9◊✲ㄢ㢟ྡ㸸㐀ᒣᖏࡢ⇕ᖺ௦Ꮫⓗ◊✲ϩ 㸦ㄢ㢟␒ྕ㸸8136㸧
ᒸᒣ⌮⛉኱Ꮫ⮬↛⛉Ꮫ◊✲ᡤ ර⸨ ༤ಙᒸᒣ⌮⛉኱Ꮫ⮬↛⛉Ꮫ◊✲ᡤ ᯈ㇂ ᚭ୸ᒸᒣ⌮⛉኱Ꮫ࣮࢜ࣉࣥࣜࢧ࣮ࢳࢭࣥࢱ࣮ 㒓ὠ ▱ኴ㑻*  *⌧ᅾࡢᡤᒓ ⵛᒣᆅ㉁ᖺ௦◊✲ᡤ
Hironobu, Hyodo, Research Insititute of Natural Sciences, Okayama University of Science
Tetsumaru Itaya, Research Insititute of Natural Sciences, Okayama University of Science
Chitaro Gouzu*, Open Research Center, Okayama University of Science, *present address*Hiruzen Institute for Geology and Chronology࡞࠸࠸ࢁ࠸ࢁ࡞ᆅ㉁Ꮫⓗせᅉ࠿ࡽ༢⣧࡞ゎ㔘ࡀ࡛┠ⓗ࡜ព⩏㐀ᒣᖏࡣࡑࢀࡀᙧᡂࡉࢀࡿ㐣⛬࡟࠾࠸࡚」㞧 ࡁ࡞࠸஦㇟ࡀከᩘᏑᅾࡍࡿࠋK-Ar ᖺ௦ἲࢆᨵⰋࡋ
࡞ᆅẆኚືࡢṔྐࢆ⤒㦂ࡍࡿࠋࡑࡢ㐣⛬࡛ᙧᡂ ࡓཎᏊ⅔࡛ࡢᨺᑕ໬ࢆ⏝࠸ࡿ 40Ar/39Ar ἲࡣࡑࡢࡼ
ࡉࢀࡓᒾ▼ࡸኚᡂࢆཷࡅࡓᒾ▼࡟ࡣࡑࡢグ㘓ࡀ ࠺࡞ሙྜ࡟ẁ㝵ຍ⇕ἲࢆ⏝࠸ࡿࡇ࡜୍࡛ᗘ㛢㙐⣔ྠ఩యࡢᣑᩓ⛣ືࡢ⤖ᯝࠊඖ⣲ศᕸ࡜ࡋ࡚ṧࡾࠊ ࡟࡞ࡗࡓᒾ▼ࡀࡑࡢᚋࠊ⇕ⓗ࣭㖔≀Ꮫⓗኚ໬ࢆ࠺ࡅ
≉࡟ᨺᑕᛶᔂቯࢆࡍࡿྠ఩య⣔࡛ࡣࡑࢀࢆ᫬ィ ࡚࠸ࡿ࠿ࢆุ᩿ࡍࡿᇶ‽ࢆᥦ౪ࡍࡿࠋ
࡜ࡋ࡚ά⏝ࡋࠊᙧᡂᖺ௦ࡸኚືᖺ௦࡜࡜ࡶ࡟ࡑ

ࡇࡢ◊✲ࡢ┠ⓗࡣ」ᩘࡢ஦㇟ࡀグ㘓ࡉࢀ࡚࠸ࡿ

ࢀࡽࡀ㉳ࡁࡓ≀⌮᮲௳ࢆ᥎ᐃࡍࡿࡇ࡜ࡀ࡛ࡁ ࡜ண᝿ࡉࢀࡿᮍ▱ࡢᒾ▼࡟ᑐࡋ 40Ar/39Ar ẁ㝵ຍ⇕ࡿࠋࡑࢀࡽࡢ᰾✀ࡢ୰࡛ 40K ࢆ⏝࠸ࡓ K-Ar ᖺ௦ ἲࢆ㐺⏝ࡍࡿࡇ࡜࡟ࡼࡾ⢭⣽࡞⇕ⓗᒚṔࡢゎᯒࢆᐃἲࡣࠊ⇕ⓗᨐ஘࡟ᑐࡍࡿ㖔≀୰ࡢ࢔ࣝࢦࣥ ⾜࠺ࡇ࡜࡟࠶ࡿࠋࡑࢀ࡟ࡼࡾᚑ᮶ࡢࡼ࠺࡟

ᐃࡋ࡚ᣑᩓ࡟㛵ࡍࡿ≀⌮ࣃ࣓࣮ࣛࢱࡀࡼࡃ◊✲ࡉࢀ࡚ ᚓࡽࢀࡓᩘ್ࢆ༢࡟ᖺ௦࡜ࡍࡿࡢ࡛ࡣ࡞ࡃࠊ࢔ࣝࢦ
࠾ࡾ㐀ᒣᖏࡢ෭༷㐣⛬࡛ K-Ar ⣔ࡀ㛢㙐ࡉࢀࡓ ࣥྠ఩యࡢᣑᩓ࡟࠾ࡅࡿ≉ᛶࢆά⏝ࡋ࡚ᒾయࡢ๐
࡜⪃࠼ࡿࡇ࡜ࡀ࡛ࡁࡿ࡚ᗘࢆ㛢Ṇᗘ࡜ᐃ⩏ࡋ ๤࣭ୖ᪼㐣⛬࠶ࡿ࠸ࡣ୍ᗘ㖔≀ࡀᙧᡂࡉࢀࡓᚋ࡛࠾

ᐃ࠿ࡽ┤᥋ⓗ࡟᥎ᐃࡍࡿࡇ࡜ࡀྍ⬟࡟࡞ࡗ ࡁࡓ஦㇟ࡢ࢖ࣥࢪࢣ࣮ࢱ࡜ࡋ࡚ᆅ㉁Ꮫⓗព࿡ࢆ࡚᫂࠸ࡿࠋࡑࡢ༙㠃ࠊ⣧⢋࡞≀⌮⣔࡛ࡣ᥎ᐃ࡛ࡁ

ࡽ࠿࡟ࡍࡿࠋ

JRR-3ࠊHR-2 ࣃ࢖ࣉࠊᆅ⌫⛉Ꮫヨᩱᨺᑕ໬ศᯒ
JRR-4ࠊTB ࣃ࢖ࣉࠊᆅ⌫⛉Ꮫヨᩱᨺᑕ໬ศᯒ

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ᐇ㦂

1500
84H2
0 m NorthApparent Age (Ma) ヨᩱ࡜↷ᑕᐇ㦂ᑐ㇟࡜ࡋࡓᒾ▼ࡣ࢝ࢼࢲ࣭ࢢࣞࣥࣅࣝᆅ㉁༊ࡢ
ࢢࣞࣥࣅࣝᒾ⬦ࡢ࿘㎶ࡢᒾ▼㸦ẕᒾ㸧࡛࠶ࡿࠋẕᒾࡢᖺ௦ࡣኚᡂᖺ௦ࡀࡼࡃ◊✲ࡉࢀࠊ㈏ධᖺ௦ࡣ
40Ar/39Ar ἲ࡜ U-Pb ἲ࡟ࡼࡗ࡚Ỵᐃࡉࢀ࡚࠾ࡾࠊ

1000
Hornblende500

Ar/ Arࡑࡢ୍⮴ࡶⰋ࠸ࠋᒾ⬦ࡢ⇕ⓗࣔࢹࣝࡣẚ㍑ⓗศᯒ

50
0
0.0

37

࿘㎶ࡢẕᒾ∦㯞ᒾ୰ࡢ㖔≀ࡢ࢔ࣝࢦࣥᣑᩓࢆ
40Ar/39Ar

0
100

39

ࡋࡸࡍ࠸ࡢ࡛ࠊ㈏ධ᫬࡟࡛ࡁࡓ⇕ኚᡂࢆ⤒㦂ࡋࡓ

Tint = 883 㼼㻌㻌㻌16 Ma

0.2

0.4ኚᡂࢆཷࡅࡓゅ㛝▼ヨᩱ㸦࢝ࢼࢲࠊ࢜ࣥࢱࣜ࢜㸧.
ࢥࣥࢱࢡࢺ࠿ࡽ 10cm ௨ෆ.

⛬ᗘࡢ⣽⢏࡟○ࡁࠊ㐀ᒾ㖔≀࡛࠶ࡿゅ㛝▼ࠊ㯮㞼ẕ࠾ࡼࡧ㛗▼ࢆࣁࣥࢻࣆࢵ࢟ࣥࢢ࡟ࡼࡾศ㞳ࡋ

2000
Apparent Age (Ma)ࡓࠋᑐ㇟࡜ࡍࡿ㖔≀ࢆ 2 ࣑ࣜᚄࡢࢻࣜࣝᏍࡀ࠶࠸
ࡓ㧗⣧ᗘ࢔࣑ࣝࢺࣞ࢖࡟ࡢࡏࠊ4 - 5 ẁ✚ࡳ࡟ࡋ࡚࣎ࣝࢺࢼࢵࢺ࡛ᅛᐃࡍࡿࠋࡇࡢヨᩱ࣍ࣝࢲࢆ
JRR-3 ࡣ⡆᫆࢔࣑ࣝᐜჾࠊJRR-4 ࡣ▼ⱥ⟶࡟┿✵ᑒධࡋࡓᚋ 0.5 ࣑ࣜཌࡢ࢝ࢻ࣑࣒࢘ࢆᕳ࠸࡚ࠊ6

Biotite

1000

39
37

ࡿࡓࡵࡢᶆ‽ᖺ௦ヨᩱ࡜ࡋ࡚ hb-3gr ࢆ୰ᛶᏊ᮰

0
20
10
0
0.0

0.2

0.4

0.6

0.8

1.0

39

Fraction of Ar releasedᐦᗘࡢ೫ࡾࡢ᭷↓ࢆ࠶ࡿ⛬ᗘホ౯࡛ࡁࡿࡼ࠺࡟ࢺ
ࣞ࢖ࡢእഃᑐゅ࡟ 2 ಶࠊ୰ᚰ࡟ 1 ಶ㓄⨨ࡋࡓࠋ

Tint = 854㼼㻌㻌㻌9 Ma500

Ar/ Ar࢖࡟ࡣᮍ▱ヨᩱࡢ௚࡟୰ᛶᏊ↷ᑕ㔞ࢆࣔࢽࢱ࣮ࡍ

84B2
0 m North1500᫬㛫↷ᑕࢆ 1 – 4 ࢧ࢖ࢡࣝ⾜ࡗࡓࠋྛ࢔࣑ࣝࢺࣞ

኱ࡁࡉ⣙ 0.5 ࣑ࣜࡢ㖔≀ヨᩱࢆ㉥እᨺᑕ

1.0

ᅗ 1 ࢢࣞࣥࣅࣝᒾ⬦࡟㈏ධࡉࢀࡓ∦㯞ᒾ୰ࡢ⇕

ヨᩱࢆࡇࡪࡋ኱ࡢ኱ࡁࡉ࡛᥇ྲྀࡋࠊ60 ࣓ࢵࢩࣗ

ᐃᐇ㦂

0.8

Fraction of Ar releasedἲ࡛ゎᯒࡍࡿࡇ࡜࡟ࡼࡾࡑࢀࡒࢀࡢ㖔≀ࡢ≉ᛶࢆㄪ࡭ࡓࠋ

ᖺ௦

0.6
39

ᅗ 2 ࢢࣞࣥࣅࣝᒾ⬦࡟㈏ධࡉࢀࡓ∦㯞ᒾ୰ࡢ⇕ኚᡂࢆཷࡅࡓ㯮㞼ẕヨᩱ㸦࢝ࢼࢲࠊ࢜ࣥࢱࣜ࢜㸧. ࢥᗘィ ࣥࢱࢡࢺ࠿ࡽ 10cm ௨ෆ.

- 349 -3-9
㻝㻜㻢

JAEA-Review 2013-039

࡟ࡼࡗ࡚
㝵ⓗ࡟

ᗘࢆࣔࢽࢱࡋ࡞ࡀࡽ㐃⥆࣮ࣞࢨ࣮࡛ẁ ࡟క࠺ὶయࡢ⛣ືࡀ㛵୚ࡋࡓ࡜⪃࠼ࡿ᪉ࡀጇᙜ࡛

ᗘࢆቑຍࡉࡏ࡞ࡀࡽ 30 ⛊㛫ຍ⇕ࡋࠊࢤࢵ ࠶ ࢁ ࠺ ࠋ ࡑ ࡢ ཯ 㠃 ࡛ ὶ య ࡟ ࡼ ࡿ ⇕ ࡢ ⛣ ື ࡣࢱ࣮࡟ࡼࡗ࡚཯ᛂᛶ࢞ࢫࢆ㝖ཤ⢭〇ࡋࡓᚋࠊᕼ࢞ permeability ࡢⴭࡋࡃప࠸⤖ᬗ㉁ᒾ▼ࡢ୰࡛ࡣ㔞
ࢫ㉁㔞ศᯒィ࡛ྛࢫࢸࢵࣉࡈ࡜ࡢ 40Ar/39Ar ᖺ௦ ⓗ࡞ᐤ୚ࡣ࠶ࡲࡾ኱ࡁࡃ࡞࠸࡜⪃࠼ࡽࢀࡿࡢ࡛ࠊ
ὶయࡣ୺࡟࢔ࣝࢦࣥࡢ⛣ື࡟㛵୚ࡋࠊᐃࢆ⾜ࡗࡓࠋ

ᗘࡀᨭ㓄ࡍࡿ㖔≀୰ࡢ࢔ࣝࢦࣥᣑᩓࡣࠊᒾ⬦ࡢ୧ഃ࡛࡯ࡰ

⤖ᯝ࠾ࡼࡧᡂᯝᐃࡋࡓゅ㛝▼࠾ࡼࡧ㯮㞼ẕࡣ㈏ධᒾ⬦ࡢ࿘ࡾ ྠ➼࡛࠶ࡿ࡜᥎

ࡉࢀࡿࠋ㐣๫࢔ࣝࢦࣥࡢࢯ࣮ࢫ

࡟ᅗ 1 ࠾ࡼࡧᅗ 2 ࡟♧ࡍࡼ࠺࡞」㞧࡞ᖺ௦ࢫ࣌ࢡ ࡣ࠾ࡑࡽࡃẕᒾ⮬య࡛࠶ࡿࡢ࡛ᒾ⬦ࡢ୧ഃ࡛ࡢᖺ
ࢺࣝࢆ♧ࡍࠋࡇࢀࡽࡣྠࡌ⇕ᒚṔࢆ⤒㦂ࡋ࡚࠸ࡿ ௦ࢫ࣌ࢡࢺࣝࡢ㐪࠸ࡣࠊὶయࡢ⤒㊰ࡢ㐪࠸࡜ࡑࡢࡢ࡛࠶ࡿ࠿ࡽ㛢Ṇᗘ࡟ᑐᛂࡋࡓྠࡌࡼ࠺࡞ࢫ࣌ ᫬㛫ⓗኚ໬࡛࠶ࡿ࡜᥎

ࡉࢀࡿࠋࢡࢺࣝࢆ♧ࡍࡇ࡜ࡀᮇᚅࡉࢀࡿࠋࢺ࣮ࢱࣝᖺ௦ࡔ ࡲ࡜ࡵ࡜ホ౯ࡅ࡟ὀ┠ࡍࢀࡤᚲࡎࡋࡶࡑࡢ㛤ࡁࡣ኱ࡁࡃ࡞ࡃᩚ  ࡇࡢ◊✲࡛ࡣ 40Ar/39Ar ᖺ௦ᐃ࡟࠾࠸࡚ࡋࡤ

ྜⓗ࡟ࡳ࠼ࡿࠋࡋ࠿ࡋ⤖ᯝࢆぢ࡚᫂ࡽ࠿࡞ࡼ࠺࡟ ࡋࡤၥ㢟࡜࡞ࡿ㐣๫࢔ࣝࢦࣥࡢཎᅉࡀẕᒾ࡟㉳ᅉࡑࢀࡽࡢࢫ࣌ࢡࢺࣝᙧ≧ࡣప㒊࡜㧗㒊࡛඲ࡃ ࡍࡿࡶࡢ࡛࠶ࡿࡇ࡜ࢆ♧ࡍࡇ࡜ࡀ࡛ࡁࡓࠋࡲࡓࡑ

␗࡞ࡿࠋࡇࡢ⌧㇟ࡣ᥋ゐ㒊㸦ࢥࣥࢱࢡࢺ㸧࠿ࡽ㏆ ࡢ⵳✚ࡢࡋ࠿ࡓ࡛ 40Ar/39Ar ᖺ௦ࢫ࣌ࢡࢺࣝࡢᙧ
࠸࡯࡝㢧ⴭ࡛࠶ࡿࠋࡲࡓᒾ⬦ࡢ㉮⾜ࡣᮾす࡛࠶ࡾࠊ ≧ࡀ኱ࡁࡃ␗࡞ࡿ⤖ᯝࢆ♧ࡋࡓࠋࡇࡢཎᅉ࡜ࡋ࡚
ᖹ㠃ࡀ໭࡟ྥ࠿ࡗ࡚ᆶ┤ࡼࡾ⣙ 20 ᗘഴ࠸࡚࠸ࡿ ὶయࡢ㛵୚ࡀ᥎ㄽࡉࢀࠊࡲࡓࡑࡢᙉᗘ࡟࠾࠸࡚ࡶ
ࡀࠊࢺ࣮ࢱࣝᖺ௦ࡔࡅ࡛࡞ࡃࠊྠࡌ㊥㞳ࡔࡅࢥࣥ ὶయࡢ⤒㊰ࡀ኱ࡁࡃᙳ㡪ࡋ࡚࠸ࡿ࡜ᛮࢃࢀࡿࠋ
ᐇ᪋ࡉࢀࡓ JRR-3, JRR-4 ࡛ࡢ 40Ar/39Ar ᖺ௦ࢱࢡࢺ࠿ࡽ㞳ࢀࡓ໭ഃ࡜༡ഃࡢヨᩱ࡛㯮㞼ẕࠊゅ㛝▼ࡢᖺ௦ࢫ࣌ࢡࢺࣝᙧ≧ࡀ඲ࡃ␗࡞ࡿ஦ࡀ☜ㄆ ᐃ࡛ࡣࠊᖸ΅ྠ఩యࡢ⿵ṇ್ࡣ(38Ar/39Ar)K ࡢ್ࢆࡉࢀࡓࠋ㝖ࡁ๓ᅇࡢ◊✲࡜ྠᵝࡲࡔᐇ㦂ࡈ࡜࡟ㄗᕪࡀ኱ࡁ

ࡇࡇ࡟ࡍ࡭࡚ࡢࢹ࣮ࢱࢆ♧ࡍࡇ࡜ࡀฟ᮶࡞࠸ࡢ ࠸ࠋࡇࢀࡀ‽ഛࡋࡓᶆ‽ヨᩱ࡟㉳ᅉࡍࡿࡶࡢ࡞ࡢ
࡛ヲࡋ࠸㆟ㄽࡣูࡢᶵ఍࡜ࡍࡿࡀࠊᒾ⬦ࢆ࡬ࡔ࡚ ࠿ࠊཎᏊ⅔ࡢ❧ࡕୖࡆࡈ࡜ࡢ୰ᛶᏊ᮰ᐦᗘࡢࡤࡽ
ࡓ໭࡜༡ࡢ㯮㞼ẕࡢᖺ௦ࢫ࣌ࢡࢺࣝࡢ㐪࠸ࡣᒾ⬦ ࡘࡁ࡟ࡼࡿࡶࡢ࠿ࡣุ᩿ࡀࡘ࠸࡚࠸࡞࠸ࠋJRR-4
ࡢᖹ㠃ࡢ୧ഃ࡟⥺ᑐ⛠ࢆసࡾฟࡍ⇕ఏᑟࣉࣟࢭࢫ ࡛ࡣ࢝ࢻ࣑࣒࢘ࢆヨᩱ࡟ᕳ࠸࡚⇕୰ᛶᏊࢆ࠶ࡿ⛬ࡔࡅ࡛ᙧᡂࡉࢀࡓ࡜ࡣ⪃࠼࡟ࡃࡃࠊ࠾ࡑࡽࡃࡑࢀ

ᗘ㐽ⶸࡍࡿࡇ࡜ࡀ࡛ࡁࡿࠋヨᩱࡢᨺᑕᛶᙉᗘࡣ࢝

3-9- 350 -

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JAEA-Review 2013-039

ࢻ࣑࣒࢘ࢆᕳ࠸࡚࠸࡞࠸ࡶࡢ࡜ẚ࡭ࡿ࡜ⴭࡋࡃప グ㍕ࡋ࡚࠸࡞࠸ࡇ࡜ࢆ࠾ルࡧ࠸ࡓࡋࡲࡍࠋ
ࡃࠊࡲࡓᖸ΅ྠ఩యࡢ࡬ࡢᙳ㡪ࡶపῶ࡛ࡁࡿ஦ࡀ Ⓨ⾲ㄽᩥ㸦40Ar/39Ar ἲࢆ⏝࠸ࡓࡶࡢ.
ࢃ࠿ࡗࡓࠋᖺ௦ᶆ‽ヨᩱࡢ J-್ࡢࡤࡽࡘࡁ࠿ࡽホ┤᥋ⓗ㛵୚ࡣ 4 ࡜ 5 ࡢࡳ㸧1) Itaya, T., Hyodo, H., Tsujimori, T., Wallis, S.,
Aoya, M., Kawakami, T., Gouzu, C. (2009)
Regional-scale excess Ar wave in a Barrovian typeᖹ࠾ࡼࡧᆶ┤ศᕸࡣࡸࡸࡤࡽࡘࡁࡀ኱ࡁ࠸ࡀ࠾࠾
metamorphic belt, eastern Tibetan Plateau, Island
Arc, 18, 293-305.
ࡼࡑᩘࣃ࣮ࢭࣥࢺ࡟཰ࡲࡗ࡚࠸ࡿࠋࡋ࠿ࡋಶࠎࡢ
2) Miki, M., Taniguchi, A., Yokoyama, M., Gouzu,
ヨᩱࡢࡤࡽࡘࡁ࡛ẚ㍑ࡍࡿ࡜ 10 ࣃ࣮ࢭࣥࢺࢆ㉺C., Hyodo, H., Zaman. H. and Otofuji, Y. (2009)౯ࡋࡓ୰ᛶᏊ᮰ࡢᆒ㉁ᛶ࡛ࡣࠊྠࡌ↷ᑕ᮲௳࡛Ỉ

Paleomagnetism࠼ࡿࡶࡢࡶ࠶ࡾࠊ௒ᚋࡢ᳨ウㄢ㢟࡛࠶ࡿࠋProterozoic࡞࠸ࡶࡢࡀ࡯࡜ࢇ࡝࡛࠶ࡿࠋࡑࢀࡣ↷ᑕᚋ 3 ࣨ᭶ 3)ᐃࡑࡢࡶࡢ࡟

᫬㛫ࡀ࠿࠿ࡿࡇ࡜ࠊ࣐ࢩࣥࢱ࢖࣒࡞࡝࡟ࡼࡿࠋᚑ
4)
ࡗ࡚ከࡃࡢ
࡟

ᐃࡣᖹᡂ 19-20 ᖺᗘࡢヨᩱࢆ 1 ᖺᚋᐃࡍࡿࡼ࠺࡞ࢫࢣࢪ࣮ࣗࣝ࡜࡞ࡾࠊⓎ⾲ࡢᶵ 5)఍ࢆᚓ࡚࠸࡞࠸ࡶࡢࡀከ࠸ࠋ௒ᚋᏛ఍ࠊㄽᩥㄅ࡞
6)

࡝࡟Ⓨ⾲ࡋ࡚࠸ࡃணᐃ࡛࠶ࡿࠋ
◊✲ࡢᛶ᱁ୖࠊྠࡌᖺᗘෆ࡟ලయⓗᴗ⦼ࢆሗ࿌ࡍ
ࡿࡇ࡜ࡣⴭࡋࡃᅔ㞴࡛࠶ࡿࠋ௒ᅇࡢඹྠ฼⏝࡟ࡼ6)ࡿ↷ᑕᐇ㦂ࡢ┤᥋ⓗ⤖ᯝ࡜ࡣ↓㛵ಀ࡛ࡣ࠶ࡿࡀࠊ
ཧ⪃࡜ࡋ࡚ 19-20 ᖺᗘ௨๓࡟ி㒔኱ᏛཎᏊ⅔࡛⾜ࡗࡓ୰ᛶᏊ↷ᑕ࡟ࡼࡿ 40Ar/39Ar ᖺ௦

doleritegeochronology
dyke

from

of

the

southwest

Greenland: indication of low paleointensity, ,ࡇࡢሗ࿌࡛ࡢ⤖ᯝࡣࡲࡔබࡢሙ࡛Ⓨ⾲ࡉࢀ࡚࠸௨ୖࡢ෭༷ᮇ㛫ࢆ࠾ࡃᚲせᛶࡸࠊ

and

7)

ᐃࡢ⤖ᯝ

࠿ࡽⓎ⾲ࡉࢀࡓㄽᩥࢆ௨ୗ࡟ཧ⪃ࡢࡓࡵ࡟ิᣲࡍ
ࡿࠋࡇࡢ࠺ࡕ 4 ࡜ 5 ࡢࢹ࣮ࢱ࠾ࡼࡧゎ㔘࡟ࡘ࠸࡚ཎᏊຊᶵᵓ᪋タ฼⏝ඹྠ◊✲ࡢ⤖ᯝࢆ୍㒊౑⏝ࡋ࡚࠸ࡿࠋⴭ⪅ࡢ୙ぬ࡟ࡼࡾㅰ㎡࡟᪋タ฼⏝ࡢ௳ࢆ- 351 -

Geophysical Journal International, 179, 18-34.
Nuong, N.D., Itaya, T., Hyodo, H. and Yokoyama,
K. (2009) K-Ar and 40Ar/39Ar phengite ages ofSanbagawa schist clasts from the Kuma Group,
central Shikoku, SW Japan. Island Arc, 18,282-292.
Hyodo, H. (2008) Laser Probe 40Ar/39Ar dating:History and development from a technicalperspective. Gondwana Research 14, 609-616.
ර⸨༤ಙ (2008) ◊✲⅔JRR3࡛ᚓࡽࢀࡓJ್࠾ࡼࡧᖸ΅ྠ఩య⿵ṇ್, ᒸᒣ⌮⛉኱Ꮫ⮬↛⛉Ꮫ◊✲ᡤ◊✲ሗ࿌ ➨34ྕ, 39-42.ෆ㔝㝯அ࣭ᕝᮧಙே࣭㒓ὠ▱ኴ㑻࣭ර⸨༤ಙ
(2008) ᰿⏣ⱱᖏ♟ᒾ࠿ࡽᚓࡽࢀࡓྵࢨࢡࣟ▼Ἶ㉁∦ᒾ♟ࡢⓑ㞼ẕ40Ar/39Arᖺ௦. ᆅ㉁Ꮫ㞧ㄅ
114 (6) 314-317.
Kawamura, M., Uchino, T., Gouzu, C. and Hyodo,
H. (2007) 380 Ma 40Ar/39Ar ages of the high-P/Tschists obtained from the Nedamo Terrane,
Northeast Japan. Journal of Geogical Society ofJapan, 113, 492-499.
Nakatsukasa, M., Sawada, Y., Sakai, T., Hyodo,
M., Hyodo, H., Itaya, T., Nakaya, H., Saegusa,
H., Mazurier, A., Saneyoshi, M., Tsujikawa, H.,
Yamamoto, A., Mbua, E. (2007) A new Late
Miocene great ape from Kenya and its implications
for the origins of African great apes and humans.
Proceedings of National Academy of Science USA,104, 19220-19225.

3-9

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JAEA-Review 2013-039

3-10㖔▼ヨᩱࢆྵࡴ᪥⏝ရࡢ 6P*G ẚἲ࡟ࡼࡿ⏘ᆅྠᐃ࡜㖔▼ࡢయ⣔໬
3URGXFWLRQLGHQWLILFDWLRQPHWKRGRIFRQVXPHUSURGXFWVLQFOXGLQJRUHVDVUDGLDWLRQVRXUFHVDQG
FODVVLILFDWLRQRIRUHVE\6P*GUDWLRVྂ⏣ ᝋᏊ㸦࠾ⲔࡢỈዪᏊ኱Ꮫ኱Ꮫ㝔㸧ࠊ⟪㍯ࡣࡿ࠿㸦ᮾிឿᜨ఍་⛉኱Ꮫ㸧(WVXNR)XUXWD2FKDQRPL]X8QLYHUVLW\*UDGXDWH6FKRRO+DUXND0LQRZD7KH-LNHL8QLYHUVLW\6FKRRORI0HGLFLQH୍⯡ᾘ㈝㈈ࡢᨺᑕ⥺※ࡣࠊࢺ࣒ࣜ࢘㸦7K㸧࢘ࣛ࠙◊✲┠ⓗࠊព⩏ࠚ  ኳ↛ᨺᑕᛶྠ఩ඖ⣲ࢆྵࡴ᪥⏝ရࡣᨺᑕᛶࢥࣥ

ࣥ㸦8㸧ࡀ࡯࡜ࢇ࡝࡛࠶ࡿࠋࡇࢀࡽᨺᑕ⥺※࡜ࡋ࡚ࠊࢩ࣮࣐ࣗࣉࣟࢲࢡࢺ 5&3 ࡜࿧ࡤࢀࠊᗈࡃ⏕άᅪෆࣔࢼࢨ࢖ࢺ㖔▼ࠊࣂࢫࢺࢿࢧ࢖ࢺ࡞࡝ᩘ✀㢮ࡀࠕ࢞

࡟ὶ㏻ࡋ࡚࠸ࡿࠋ5&3 ࡣᨺᑕ⥺ࢆᨺฟࡋ࡚࠾ࡾࠊᨺ

࢖ࢻࣛ࢖࡛ࣥࠖࡣࠊᣦᐃཎᮦᩱ࡜ࡋ࡚ᣲࡆࡽࢀ࡚

ᑕ⥺※ࡢ⃰ᗘࡢ㧗࠸ 5&3 ࡣእ㒊࣭ෆ㒊⿕ࡤࡃࡢཎ࠸ࡿࠋࡋ࠿ࡋࠊࡇࢀࡣ⛉Ꮫⓗ᰿ᣐࡀ࠶ࡿࢃࡅ࡛ࡣ

ᅉ࡜࡞ࡿ༴㝤ᛶࡀ࠶ࡿࠋᮏ◊✲ࡣࠊ㖔▼⏤᮶ᡂศ࡞࠸ࠋ

ࢆྵࡴ 5&3㸦1250㸧ࡢཎᮦᩱࢆࠊ༶ⓎȚ⥺ᨺᑕ໬ศ

7K8 ࢆከࡃྵࡴ㖔▼ࡣࠊᕼᅵ㢮ඖ⣲ࢆྠ᫬࡟ከ

ᯒἲ㸦3*$$㸧࡟ࡼࡾ᥎ᐃࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡍࡿࠋ

ࡃྵࢇ࡛࠸ࡿࡇ࡜ࡀከ࠸ࠋ1250 ࡢ 3*$ ࡟ࡼࡿ㠀◚  5&3 ࡢᨺᑕ⥺※ࡣࠊேᕤ࣭ኳ↛ࡢᨺᑕᛶྠ఩ඖ

ቯศᯒ࡟ࡼࡾࠊ6P*G ࡢࡳࡀ ᐃฟ᮶ࡿࡇ࡜࠿ࡽࠊ

⣲ࡢ࡝ࡕࡽࡶ᭷ࡾ࠺ࡿࡀࠊ㏆ᖺࢳࢱࣥ࡞࡝ࡢ㖔▼୍⯡ᾘ㈝㈈࡜ࡋ࡚ࡢ 1250 ࡢཎᩱ㖔▼ࡢ᥎ᐃ࡟ࡣ

ࢆ⏝࠸ࡓ⏘ᴗ⏺࡟࠾ࡅࡿኳ↛ᨺᑕᛶྠ఩ඖ⣲ࡢྵ

3*$$ ࡀ᭷ຠ࡛࠶ࡿ࡜⪃࠼ࡽࢀࡿࠋ᪥ᮏᅜෆ࡟ධࡗ

᭷ࡀసᴗ⪅ࠊᗫᲠ≀ᴗ⪅ࡢ⿕ࡤࡃ࡟ࡘ࡞ࡀࡾࠊ኱

࡚ࡁ࡚࠸ࡿᨺᑕ⥺※ࡣࠊከᒱ࡟ࢃࡓࡗ࡚࠸ࡿ࡜ࡣ

ࡁ࡞♫఍ၥ㢟࡜࡞ࡗ࡚ࡁ࡚࠸ࡿࠋࡇࡢࡼ࠺࡞ኳ↛⪃࠼࡟ࡃ࠸ࠋᮏἲ࡟ࡼࡾཎᮦᩱ㖔▼ࢆ≉ᐃࡍࡿࡇᨺᑕᛶྠ఩ඖ⣲ࢆከࡃྵࡴཎᮦᩱ㸦㖔▼㸧ࠊ୰㛫〇࡜ࡀྍ⬟࡜⪃࠼ࡽࢀࡿࠋཎᮦᩱ㖔▼ࡀ≉ᐃࡉࢀࡓရ ࡸ ୍ ⯡ ᾘ ㈝ ㈈ ࡣ 1250 1DWXUDOO\ 2FFXUULQJሙྜࠊ㍺ධ᫬ࡢὀពႏ㉳࡟ࡘ࡞ࡀࡾࠊ୙ᚲせ࡞ 5&3

5DGLRDFWLYH0DWHULDOV ࡜࿧ࡤࢀࠊࡑࡢ೺ᗣᙳ㡪ࡢ⏕άᅪ࡬ࡢ౵ධࢆ㜵ࡄࡇ࡜ࡀྍ⬟࡜࡞ࡿ࡜⪃࠼ࡣୡ⏺ⓗ࡞ၥ㢟࡜࡞ࡗ࡚ࡁ࡚࠸ࡿࠋ,$($:+2 ࡞࡝ࡽࢀࠊࡇࡢព⩏ࡣ኱ࡁ࠸ࠋ

ࡀ 1250 ࡢつไࢆ᳨ウࡋ࡚࠸ࡿ࡜ࡇࢁ࡛࠶ࡿࠋ᪥ᮏ

࠙ィ⏬࡜㐙⾜᪉ἲࠚ࡟࠾࠸࡚ࡶࠕ࢘ࣛࣥཪࡣࢺ࣒ࣜ࢘ࢆྵࡴཎᮦᩱࠊ

㸦ᮏ◊✲ィ⏬ࡣࠊᖹᡂ  ᖺᗘ࡟ྂ⏣ࡀ⾜ࡗࡓࠊ3*$$〇ရ➼ࡢᏳ඲☜ಖ࡟㛵ࡍࡿ࢞࢖ࢻࣛ࢖ࣥࠖࡀ⟇ᐃࢺࣛ࢖࢔࣮ࣝࣘࢫ᫬࡟ 1250 ࡛࠶ࡿࠕ࣑࣍ࣝࢩࢫ໬⢝ࡉࢀࡓࠋࡋ࠿ࡋࠊ᪥ᮏࡢࠕ࢞࢖ࢻࣛ࢖ࣥࠖࡣ 1250

ရࠖ࠿ࡽᚓࡽࢀࡓ⤖ᯝ࡟ᇶ࡙ࡁࠊィ⏬ࡋࡓࡶࡢ࡛࠶

ཎᮦᩱࡸ୍⯡ᾘ㈝㈈➼ࡢ〇㐀஦ᴗ⪅ࢆᑐ㇟࡜ࡋࡓ

ࡿࠋ㸧ࡶࡢ࡛࠶ࡾࠊᨺᑕᛶ≀㉁ࡀῧຍࡉࢀࡓ୍⯡ᾘ㈝㈈ࡑࡢࡶࡢࡢᏑᅾࢆྰᐃࡍࡿࡶࡢ࡛ࡣ࡞ࡃࠊࡇࡢⅬ ⬺⮯ᮦࠊ⇞㈝ྥୖᮦࠊ࣐࢖ࢼࢫ࢖࢜ࣥ〇ရ࡞࡝ࡀ (8 ࡢࠕῧຍ⚗Ṇࠖ࡜ࡣ኱ࡁࡃ␗࡞ࡗ࡚࠸ࡿࠋࡇ
ࡢࡓࡵࠊ௒ᚋࡶ⏕άᅪෆ࡟ࡣࠊᨺᑕ⥺ࢧ࣮࣋࢖࣓
࣮ࢱࡀ኱ࡁࡃ཯ᛂࡍࡿࡼ࠺࡞ᨺᑕ⬟ࡢᙉ࠸୍⯡ᾘ㈝㈈ࡀᏑᅾࡋ⥆ࡅࡿࠋࡢከࡃࡢ୍⯡ᾘ㈝㈈ཬࡧ⏘ฟᅜࠊᆅᇦࡢ᫂ࡽ࠿
࡞㖔▼ᶆᮏ࡞࡝ࡢ 1250 ࢆヨᩱ࡜ࡋࠊ༙ᑟయ᳨ฟ
ჾ࡟ࡼࡿȚ⥺ࢫ࣌ࢡࢺࣝࡢ

ᐃ࡟ࡼࡾࠊࡑࡢ

7K8 ➼ࡢᨺᑕ⬟⃰ᗘࢆồࡵࡿࠋ-55 3*$$ ༶ⓎȚ⥺ᨺᑕ໬ศᯒ⿦⨨ࠊᨺᑕ໬Ꮫࠊ
31 ୰ᛶᏊᨺᑕ໬ศᯒࠊᨺᑕ໬Ꮫ

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 ࡇࢀࡽヨᩱࢆ  ᅇࡢ 3*$$ ࡟ࡼࡾศᯒࡋࠊヨᩱ୰࡟ྵࡲࢀࡿ 6P*G ࡣࠊࡑࡢከࡃࡀ୍┤⥺ୖ࡟㞟ࡲࡾࠊ≉ู࡞㛵ಀࢆ♧ࡋࡓࠋᖹᡂ  ᖺᗘ௨㝆ࠊࡇࡇ࡟㖔▼ࡢ 6P*G ࡢᨺᑕ⬟ࢆồࡵࡿࠋ 㸯㸬ཬࡧ㸰㸬ࡢ⤖ᯝࢆᅗ♧ࡍࡿࡇ࡜࡟ࡼࡾࠊ7K8࡟ᑐࡍࡿ *G6P ࡢ㛵ಀࢆồࡵࡿࠋ

ヨᩱࢆຍ࠼ࠊఱࡽ࠿ࡢഴྥࡀᚓࡽࢀࡿ࠿ࠊ࠶ࡿ࠸ࡣ
᭦࡞ࡿඖ⣲࡟ࡼࡿ  ḟඖࢢࣛࣇ࡟ࡼࡾゎᯒࡍࡿᚲせࡀ࠶ࡿ࠿ࢆぢᴟࡵ࡚࠸ࡿ࡜ࡇࢁ࡛࠶ࡿࠋ

,1$$ ࢆ⏝࠸ࡓᨺᑕ໬࡟ࡼࡾࠊ6P*G ௨እࡢඖ⣲࡟ࡼࡿయ⣔໬ࡀྍ⬟࡛࠶ࡿ࠿ྰ࠿ࢆ᥈ࡿࠋ

࠙ᡂᯝ࡟ᑐࡍࡿホ౯ࠚ+ ᖺᗘࠊᨺᑕ໬Ꮫウㄽ఍࡟࠾࠸࡚ࠊཱྀ㢌Ⓨ⾲ࢆ࠙ᡂᯝ࠾ࡼࡧ௒ᚋࡢ᪉㔪ࠚ⾜ࡗࡓࠋࡑࡢ⤖ᯝࠊ; ⥺ゎᯒࡣ⾜ࡗ࡚࠸ࡿ࠿ࠊ

3*$$ ᅇ࡜ࠊ㏣ຍ࡛࠾ㄆࡵ࠸ࡓࡔ࠸ࡓ ,1$$ ᅇࢆ⾜ヨᩱ࡜ࡋ࡚࠸ࡿ 1250 ࠿ࡽࡢ⿕ࡤࡃ⥺㔞ホ౯ࢆ⾜ࡗࡗࡓࠋࡋ࠿ࡋࠊ㖔▼➼ࡢᶆᮏヨᩱࡣࠊ⤖ᯝ࡜ࡋ࡚ᖹ

࡚࠸ࡿ࠿ྰ࠿ࠊ1250 ࡟㛵ࡍࡿ୺ᙇࡀ࠶ࡗࡓࡽ⪺࠿ᡂ  ᖺ  ᭶୰᪪࡟ᡭඖ࡟ᒆ࠸ࡓࡓࡵࠊᖹᡂ  ᖺᗘࡏ࡚࡯ࡋ࠸ࠊ௒ᚋࡢ᪉㔪ࡢ㉁ၥࢆ࠸ࡓࡔ࠸ࡓࠋ

ෆ࡟㐙⾜࡛ࡁࡓ

ᐃࡣ௨ୗࡢ㏻ࡾ࡜࡞ࡾࠊᖹᡂ ࡣ࠸ࡃࡘ࠿ࡢヨᩱ࡟ࡘ࠸࡚ࡣ⾜ࡗ࡚࠾ࡾࠊ௒ᚋࡶ᳨

ᖺᗘ௨㝆࡟ᨵࡵ࡚ᐇ㦂ィ⏬ࢆᥦฟࡋࠊ࠾ㄆࡵ㡬࠸ࡓࠋウࡋ࡚࠸ࡿࡇ࡜ࠊࡣ඲࡚࡟ࡘ࠸࡚⿕ࡤࡃ⥺㔞ホ౯㸯㸬 ✀㢮ࡢ୍⯡ᾘ㈝㈈ 1250 ࠾ࡼࡧ㖔▼ヨᩱࡢᨺࢆ⾜࠸ࠊ㏻ᖖࡢ౑⏝ᙧែ࡛ࡣ୍⯡බ⾗࡟ᑐࡍࡿ⿕ࡤᑕ⬟ ᐃ㸦࠾Ⲕ኱ࠊ+3*H㸧ࡃ㝈ᗘࢆ㉸࠼ࡿࡇ࡜ࡣ࡞࠸᪨ࢆሗ࿌ࠊࡣࠕṇᙜᛶࠖ㸰㸬 ✀㢮ࡢ୍⯡ᾘ㈝㈈ 1250 ࠾ࡼࡧ୍㒊㖔▼ヨᩱࡢヰࢆࡉࡏ࡚㡬ࡁࠊࡣ⏘ᆅࡢุ᫂ࡋ࡚࠸ࡿࣔࢼࢨࡢ 㹼 ᅇࡢ 3*$$࢖ࢺ࡟⤠ࡾ 3*$$,1$$ ࢆ⾜࠺ணᐃࢆ㏙࡭ࡓࠋᐃ㸱୍㒊ࡢ୍⯡ᾘ㈝㈈࡜㖔▼ヨᩱࡢ  ᅇࡢ ,1$$ᐃ࠙௒ᚋࡢ᪉㔪ࠚ ᚓࡽࢀࡓᨺᑕ⬟ࢆ⾲㸯㸹୍⯡ᾘ㈝㈈ S㸱 ࠊ⾲㸰㸹ᮏㄢ㢟ࡣࠊ㐙⾜ྍ⬟࠿ࡶྵࡵࠊ༢ᖺᗘࡢ⏦ㄳ࡜ࡋ㖔▼ヨᩱ࡜ࡋ࡚ḟ࣮࣌ࢪ S㸱㹼 ࡟グࡋࡓࠋࡉࡽ࡟ࠊ

ࡓࡀࠊྍ⬟࡛࠶ࡿ࡜ࡢឤゐࢆᚓ࡚ࠊ+ ᖺᗘࡢ⥅3*$$ ࠿ࡽᚓࡽࢀࡓ୍⯡ᾘ㈝㈈୰ࡢ *G ࡜ 6P ࡢ㛵ಀᅗ⥆ㄢ㢟࡜ࡋ࡚⏦ㄳࡋࠊ⥅⥆ࡋ࡚࠸ࡿࠋ ࢆ㹮㸲࡟グࡋࡓࠋ࠙ᡂᯝࡢබ⾲ࠚ +3*H ࡟ࡼࡿȚ⥺ ᐃ࡟ࡼࡾồࡵࡓ 7K ࡜ 8 ࡢ㛵ಀᖹᡂ  ᖺ࡟㛤ദࡉࢀࡿ $VLD3DFLILF6\PSRVLXPRQ

࠿ࡽࡣࠊ7K ࡶࡋࡃࡣ 8 ࡀከ࠸ 1250 ࡢᏑᅾ࡜ࠊ7K!8

5DGLRFKHPLVWU\̓ ࡟࠾࠸࡚Ⓨ⾲ࡍࡿ࡜࡜ࡶ࡟ࠊࡑ

ࡢ 1250 ࡢᏑᅾࡀ᫂ࡽ࠿࡜࡞ࡗࡓࠋࡋ࠿ࡋࠊ㖔▼ヨᩱ

ࡢ 3URFHHGLQJV ࡜ࡋ࡚ -RXUQDO5DGLRFKLPLFD$FWD࡜ࡢ┦㛵㛵ಀࢆ 7K8 ࡢ㛵ಀࡢࡳ࠿ࡽぢฟࡍࡇ࡜ࡣࠊ

࡟ᢞ✏ணᐃ࡛࠶ࡿࠋ

ண᝿㏻ࡾ୙ྍ⬟࡛࠶ࡗࡓࠋ୍᪉ࠊ୍⯡ᾘ㈝㈈ 1250

3-10










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JAEA-Review 2013-039

⾲ 1 㻌 㻌 㻌 㻌 㻌 㻌 㻌  ✀㢮ࡢ 5&3 1250 ࡟ྵࡲࢀࡿᨺᑕ⬟⃰ᗘ㻌 

Code
1
2
3
4
5
6
7
8
9
10
11
12
13

NORM
㻌 㻌 㻌 Kinds: Name
Jell-1Liquid (red)CreamToiletry
Face powder
Jell-2LiquidToothpaste
Bedrock-bath (red)Spring-bath Bedrock-bath (white)
powderBakeliteRa spring
Gas lantern
mantle14

Car goods

15
16
17
18
19
20
21
22

Deodorant
Pillow
Wall-paper
Ornament
Cloth

Effect clamedby maker

Hormesis

Minus-ionHealthy
Relax and healthy

Lightning
Mileage
improvement

Shoes-box
Foot deodorantRatio of
Th/U
2.7×100
5.4×100
2.9×100
5.2×100
2.7×100
1.7×10-1
2.2×10-1
6.8×100
5.6×100
6.3×101
1.3×100
4.1×101
5.0×101

2.0×100

4.6×100

4.3×10-1

2

1

8.0×100
9.9×101
6.0×100
4.2×100
5.8×100
1.0×101
7.2×10-1
1.5×100

1.7×10
1.6×1021.2×102
4.1×100
8.1×102
1.1×100
1.0×10-2
1.5×10-2

Deodorant

BraceletUnder wear
T-shirtWide stomach band

Concentration(Bq/g)
ThU
4.1×101
1.5×1011
2.1×10
3.9×1001
2.1×10
7.1×100
6.8×101
1.3×1011
4.1×10
1.5×101
3.0×10-2
1.7×10-1
3.4×10-3
1.5×10-2
1.3×103
1.9×102
1.3×1032.1×102
5.4×103
8.6×101
2.6×10-1
2.0×10-1
1.7×1024.2×100
2.9×102
5.8×100

Relax and healthy
Minus-ion
Hormesis
Detoxification
Minus-ion
Minus-ion

2.1×10
1.6×100
2.0×101
9.9×10-1
1.4×102
1.1×10-1
1.5×10-2
9.5×10-3

Additives specified in the label(Specification)
Zirconium Oxides
Tourmaline
Xenotime
Dolomite, mica, Si and so on(unknown)
Tourmaline
Tourmaline(Hearsay information: Monazite
from China)(Rn spring)(Ra powder)Th ( Canada patent)Th ( China patent)
Mineral (unknown)(China patent ; brown)
Monazite
Mineral (unknown)
Mineral (unknown)
Mineral (unknown)(The name is “monazu-bracelet”.)
Ge
Mineral (unknown)
Tourmaline⾲     ✀㢮ࡢ㖔▼ࠊ㖔≀ࠊ◁࡟ྵࡲࢀࡿࢺ࣒ࣜ࢘ࠊ࢘ࣛࣥ⃰ᗘ
Ore

2

Australia Perth

Concentration (Bq/g) Ratio
Specification
Th
U
Th/U
2
2
-1 TiO 䠄Natural Rutile䠅
5.4×10
3.0×10
1.6×102
2.8×102 2.2×102 1.3×100 FeTiO3(Ilmenite䠅

3
4
5
6
7

South Africa Richards Bay
Vietnam
Australia Perth
Australia Perth
Canada1.7×1022.3×1022.3×102
9.1×103
1.3×103

7.4×101
1.6×102
5.3×101
1.7×103
5.4×1022.2×100
1.5×100
4.4×100
5.5×100
2.3×100

8India

6.2×104

7.5×103

9India

7.1×104

3

6.4×108.2×100 TiO2, FeTiO3
1.2×101 TiO2, FeTiO3Australia

5.9×10-1

2.7×100
0

Code
1

10

Kinds

Ore

Sand

Name

Ti-ore*11

Zr-sand*

Producer and field
South Africa Richards Bay

Australia (West coast)-1

5.5×10

2.5×10

12

Pakistan

2.0×100

7.2×100

13

Pakistan

1.4×101

5.7×101

Sri Lanka

1.7×101

7.1×101

Australia Northern Territory-1

3.3×100

3.5×10

Malawi Rift Mineral Province

9.0×100

5.6×101

-1

0

11

14
15

Mineral Zircon

16

TiO2䠄Natural Rutile䠅
TiO2䠄Natural Rutile䠅
FeTiO3(Ilmenite䠅
FeTiO3(Ilmenite䠅
TiO2䠄Natural Rutile䠅

2.2×10-1 ZrO2䞉SiO2䠖ZrSiO4
2.2×10-1 ZrO2䞉SiO2䠖ZrSiO4
2.8×10-1 ZrO2䞉SiO2䠖ZrSiO4
2.4×10-1 ZrSiO4 Red
2.4×10-1 ZrSiO4 Red
9.4×10-2 ZrSiO4 Yellow
1.6×10-1 ZrSiO4 Red
1.4×10-1 ZrSiO4 Red

17

Tanzania Mabumbi

8.0×1018

Pakistan North West Province

9.5×100

5.8×10-

Pakistan

4.8×101

6.7×10-1

Pakistan

5.0×101

4.2×10-1

2.7×103

2.9×102

Canada Ontario

2.5×1032

3.5×10Brazil Tocantis
Unknown䠉1
Unknown䠉2
Unknown䠉3
Unknown䠉4

4.0×1024.2×1010

6.1×10
2.9×10-1
3.6×10-1
2.8×10-1-1

9.7×10
4.5×10-1
4.4×10-1
4.7×10-1

9.5×100 ex.(Ce,La,Nd,Th)PO4
6.3×100 ex.(Ce,La,Nd,Th)PO4
6.5×10-1 ex.(Ce,La,Nd,Th)PO4
8.3×10-1 ex.(Ce,La,Nd,Th)PO4
5.9×10-1 ex.(Ce,La,Nd,Th)PO4

6.5×10-1

5.0×10-1

1.3×100 Sold under the name of "Ra ore"

19

Mineral Bastnesite

20
21
22

America Colorado
Mineral Monazite

23
24
25
26
27
28*2

Ore

Monazite

Monazite(+Xenotime) Iran(Ce):Ce(CO3)F
7.2×101 (Ce):Ce(CO3)F
1.2×101 (Ce):Ce(CO3)F
9.4×100 ex.(Ce,La,Nd,Th)PO4
7.2×100 ex.(Ce,La,Nd,Th)PO43-10- 354 -

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JAEA-Review 2013-039

⾲ 
Ore
Code
29

Kinds

30

(Beach)Monazite
Sand

31

Name

37

1.3×10

4.2×10

2.9×102

5.8×101

India Thengapattanam-3

2.7×102

5.6×101

5.0×100 (Ce,La,Nd,Th)PO4
4.9×100 (Ce,La,Nd,Th)PO4

India Thengapattanam-4

2

7.5×101

Brazil Bahia
BrazilPakistan North West Province
Brazil1

6.8×10
5.0×101
1.9×101
2.9×1041

1.8×101.1×101
8.0×101
3.2×103

Tourmaline (powder) China, South Africa and Brazil

1.3×10-1

2.0×100

2

4

Mineral Xenotime

OreSpecification

India Thengapattanam-2

5.6×10

3.6×10

38
39

1

Ratio
Th/U

1

32
33
34
35
36

Concentration (Bq/g)
Th
U

Producer and field
India Thengapattanam-1

0(Ce,La,Nd,Th)PO4

4.9×100 (Ce,La,Nd,Th)PO4
3.9×100 YPO4
4.5×100 YPO4
2.4×10-1 YPO4
8.9×100 YPO4
6.5×10-2 NaX3Al6(BO3)3Si6O18(OH)4, X=Al,Fe,M
1.1×10-2 (Y,Ca,Fe,Th)(Ti,Nb)2(O,OH)6
8.0×100 Ca(Ce,La,Y,Th)(Al,Fe,Mg)3OH(SiO4)3

Aeschynite
Canada Bandcroft
1.5×10
1.6×10Allanite
Brazil Minas Gerais
7.4×103 9.3×101
Allanite(+Zircon)
Korea
40*2
1.1×10-1 8.6×10-2 1.3×100 Sold under the name of "Ge ore"
41
Betafite
Madagascar Antsirabe
1.1×104 5.8×10-2 1.5×105 (Ca,Na,U)2(Ti,Nb,Ta)2O6(OH)42Davidite
Kazakhstan Qaraghandy Oblysy 2.2×102 5.5×102 4.0×10-1 (Ce,La)(Y,U,Fe2+)(Ti,Fe3+)20(O,OH)38
43
Euxenite
Brazil Espirito Santo
8.0×102 1.9×104 4.3×10-2 (Y,Ca,Ce,U,Th)(Nb,Ta,Ti)2O6
44 Mineral Euxenite
America Wyoming
1.0×103 2.2×104 4.7×10-2 (Y,Ca,Ce,U,Th)(Nb,Ta,Ti)2O6
3+
45
Samarskite
America Colorado
1.4×103 9.6×103 1.5×10-1 (Y,Fe ,U)(Nb,Ta)5O4
2
3-2 (Y,Fe,U)NbO
46
Samarskite
Rossiya South Ural
1.5×10
8.3×101.2×10447
Stillwellite
Tazhikistan Alayskiy
1.8×100 5.1×101 3.5×10-2 (Ce,La,Ca)BSiO5
48
Thorianite
Madagascar Taolanaro
2.3×104 8.6×103 2.6×100 ThO2
49
Uraninite
Congo Katanga
1.1×102 8.6×104 1.2×10-3 UO250
Uraninite
America New Hampshire
6.9×102 6.7×104 1.0×10-2 UO2*1; These ores and sand are used as industrial materials for paint, ink, plastic and so on. They are imported by some big companies and theirradioactivities are controlled by the companies. They are called "industrial NORM".In the industrial NORM, 3 kinds of Ti-ores were not shown in*2; The two ores of Code No. 24 and 36 were sold at a normal handcraft shop under the name of each ore shown in the Specification column.
They were analyzed by Dr. Miyawaki like as each written䚷in the Name column.



1.0E+05
1.0E+04log(Gd; ppm)

1.0E+03
1.0E+02
1.0E+01
1.0E+00㻌㻺㻻㻾㻹㻦㻌㼥㻩㻌㻜㻚㻤㻢㻜㻞㼤㻜㻚㻥㻡㻥㻠

1.0E-01
1.0E-01 1.0E+00 1.0E+01 1.0E+02 1.0E+03 1.0E+04 1.0E+05 1.0E+06
log(Sm; ppm)ᅗ       3*$$ ࡟ࡼࡾồࡵࡓ 1250 ࡟ྵࡲࢀࢀࡿ 6P ࡜ *G ࡢ㛵ಀ


3-10



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JAEA-Review 2013-039

3-11
኱Ẽ⎔ቃヨᩱ࡟࠾ࡅࡿᚤ㔞ඖ⣲ࡢᐃ㔞࡜ࡑࡢᣲື㸦ϩ㸧
Determination and behavior of trace elements
in atmospheric samples (䜔)◊✲௦⾲⪅㸸ᮏከ↷ᖾ㸦ᮾி㒔ᕷ኱ᏛཎᏊຊ◊✲ᡤ㸧◊✲༠ຊ⪅㸸ᘅ℩຾ᕫ㸦Ẽ㇟◊✲ᡤ㸧                   ᮌᕝ⏣႐୍㸦ୖᬛ኱Ꮫ⌮ᕤᏛ㒊㸧                  Teruyuki HONDA (Atomic Energy Research Laboratory, Tokyo City University)
Katsumi HIROSE (Meteorological Research Institute)
Yoshikazu KIKAWADA (Faculty of Science and Technology, Sophia University)             Ϩ㸬ࡣࡌࡵ࡟

࡛࠶ࡾࠊղAPM࡟ࡘ࠸࡚ࡣࠊྠࡌࡃᮾி㒔ᕷ኱㸦ཎ኱Ẽ⎔ቃࢆᕠࡿ≧ἣࡣࠊ18㹼19 ୡ⣖ࡢ⏘ᴗ㠉࿨௨Ꮚຊ◊✲ᡤ㸧࡟࠾࠸࡚ࠊࣁ࢖࣒࣭࢚࣎ࣜ࢘࢔ࢧࣥࣉ

᮶ⴭࡋࡃኚືࡋ࡚ࡁ࡚࠾ࡾࠊṦ࡟஧㓟໬Ⅳ⣲➼ࡢ࣮ࣛ࡟ࡼࡾ᥇ྲྀࡋࡓ㐌㛫ヨᩱ࡛࠶ࡿࠋ

ᐊຠᯝ࢞ࢫࡢᨺฟ࡟క࠺ᆅ⌫ ࡞࠾ࠊᮏ◊✲࡛ࡣᚤ㔞ඖ⣲ࡢᐃ㔞࡟ᙜヱඹྠ฼⏝ᬮ໬ࡢၥ㢟ࡣࠊᆅ⌫࡟ࡼࡿ୰ᛶᏊᨺᑕ໬ศᯒࢆ㐺⏝ࡋࡓࠋつᶍࡢㄢ㢟࡜ࡋ࡚ᥦ㉳ࡉࢀ࡚࠸ࡿࠋ ࡋ࠿ࡋ࡞ࡀࡽࠊ኱Ẽ⎔ቃࡢືែࢆṇ☜࡟ホ౯ࡍࡿ࡟ࡣᐊຠᯝ࢞ࢫࡢኚື㸦⃰ᗘୖ᪼㸧ࡢࡳ࡞ࡽࡎࠊ

ϩ㸬୰ᛶᏊᨺᑕ໬ศᯒ

ᚤ㔞ඖ⣲ࡸேᕤཬࡧኳ↛ᨺᑕᛶ᰾✀➼ࢆ⏝࠸ࡓ኱Ẽ ᮏ◊✲࡛ࡣࠊ2✀㢮ࡢヨᩱࢆ⏝ពࡋࡓࠋ⎔ቃ≀㉁ࡢ㉳※୪ࡧ࡟ᣲືࢆṇ☜࡟ᢕᥱࡋࠊホ౯ࡍඛࡎࠊ㸦1㸧඲㝆ୗ≀࡟ࡘ࠸࡚ࡣࠊձ㞵Ỉࢆྵࡴヨࡿᚲせࡀ࠶ࡿࠋ

ᩱࢆ⵨Ⓨ஝ᅛࡋࠊղᑓ⏝ࡢᐜჾ㸦V7㸧࡟ᑒධࡋࡓࠋ

ࡑࡇ࡛ᮏ◊✲࡛ࡣࠊ኱Ẽ⎔ቃࢆ᥈ࡿୖ࡛㔜せ࡜࡞

㸦2㸧APM࡟ࡘ࠸࡚ࡣࠊձࣁ࢖࣒࣭࢚࣎ࣜ࢘࢔ࢧࣥ

ࡿ㝆ୗ≀ཬࡧ኱Ẽ⢏Ꮚ≧≀㉁㸦Airborne Particulateࣉ࣮ࣛ࡟࡚▼ⱥࣇ࢕ࣝࢱ࣮࡟཰㞟ࡋࠊղ୍㒊ࢆࣃࣥMatters, APM㸧ࢆヨᩱ࡜ࡋ࡚᥇ྲྀࡋࠊࡑࢀࡽ࡟ྵࡲ

ࢳ࡛ᡴࡕᢤࡁࠊᨺᑕ໬⏝ヨᩱ࡜ࡋࡓࠋ

ࢀࡿᚤ㔞ඖ⣲୪ࡧ࡟ᨺᑕᛶ᰾✀ࢆศᯒࠊゎᯒࡋࠊࡑࡑࢀࡽࡢヨᩱ࡟ࡘ࠸࡚ࠊJRR-3 ࡢ P-3 ୪ࡧ࡟ P-1

ࡢ⤖ᯝࢆ⏝࠸࡚ࠊ኱Ẽ㝆ୗ≀୪ࡧ࡟PMࡢ㉳※ࢆゎ᫂

ࡲࡓࡣ P-2 Ẽ㏦⟶ࢆ⏝࠸࡚↷ᑕࢆ⾜࠸ࠊ㐺ᙜ࡞෭༷ࡋࠊࡉࡽ࡟ࠊ᳨ฟࠊᐃ㔞ࡉࢀࡓᨺᑕᛶ᰾✀ࡸᚤ㔞ඖ᫬㛫ࢆ⤒ࡓᚋࠊ࢔࣑ࣝࢽ࣒࢘㸦Al㸧ࠊࣂࢼࢪ࣒࢘㸦V㸧ࠊ⣲ࡢ᣺⯙࠸ࢆ㏻ࡌ࡚ࠊ኱Ẽ⎔ቃ≀㉁ࡀ࡝ࡢࡼ࠺࡟ᣲ

࣐ࣥ࢞ࣥ㸦Mn㸧➼ࡢ▷ᑑ࿨᰾✀ࡣࠊᙜ᪥ࠊཎᏊຊ

ືࡋ࡚࠸ࡿࡢ࠿ࢆ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡋࡓࠋᶵᵓ(JRR-3)࡟࡚

ᐃࡋࠊ௚ࡢ୰࣭㛗ᑑ࿨᰾✀࡟ࡘᮏ◊✲࡟౪ࡍࡿヨᩱࡣࠊ㸰✀㢮࠶ࡿࠋձ㝆ୗ≀࡟࠸࡚ࡣᮾி㒔ᕷ኱ཎᏊຊ◊✲ᡤ࡟㒑㏦ࡋࡓࠋ↛ࡿᚋࠊࡘ࠸࡚ࡣࠊ⚄ዉᕝ┴ᕝᓮᕷࡢᮾி㒔ᕷ኱㸦ཎᏊຊ◊ᮾி㒔ᕷ኱࡟࡚Ț⥺ࢫ࣌ࢡࢺ࣓ࣟࢺࣜࢆᐇ⾜ࡋࠊ⮯✲ᡤ㸧࡛᥇ྲྀࡋࡓ඲㝆ୗ≀㸦஝ᛶ㸩‵ᛶ㸧᭶㛫ヨᩱ⣲㸦Br㸧ࠊ࢔ࣥࢳࣔࣥ㸦Sb㸧ࠊࣛࣥࢱࣀ࢖ࢻ࠾ࡼࡧࢺ                                                  JRR-3 PN-1ࠊPN-2ࠊPN-3
   ᆅ⌫⛉Ꮫヨᩱᨺᑕ໬ศᯒ

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JAEA-Review 2013-039

⾲ 1 ୰ᛶᏊ↷ᑕཬࡧ࣐࢞ࣥ⥺ࡢᐃ᮲௳࣒ࣜ࢘(Th)ࠊ࢘ࣛࣥ㸦U㸧➼ࡢᚤ㔞ඖ⣲ࡢศᯒ࣭ᐃ

⏕ⓗ࡞ࡶࡢ࡞ࡢ࠿ࠊேⅭⓗ࡞ࡶࡢ࡞ࡢ࠿ヲࡋࡃ▱ࡿ㔞ࢆ⾜ࡗࡓࠋ

ࡓࡵ࡟ࠊ⃰⦰ಀᩘ࡟ࡼࡿ᳨ウࢆ⾜ࡗࡓࠋ⃰⦰ಀᩘ࡜ ↷ᑕཬࡧ ᐃ᮲௳ࢆ⾲⾲ 1 ࡟グ㍕ࡍࡿࠋࡣᐃ㔞ࡉࢀࡓඖ⣲ࡢ㉳※ࢆ▱ࡿᣦᶆ࡟࡞ࡿࡶࡢ࡛⃰⦰ಀᩘࡀ  ௨ୖ࡞ࡽேⅭⓗ࡛ࠊ ࡼࡾᑠࡉ࠸࡞ࡽ

Ϫ㸬ᡂᯝࡢᴫせ⮬↛Ⓨ⏕ⓗ࡞ࡶࡢ࡜⪃࠼ࡽࢀࡿࠋ
㸦㸯㸧ᘧ࡟⃰⦰ಀᩘ㸯㸬኱Ẽ㝆ୗ≀࡟࠾ࡅࡿᚤ㔞ඖ⣲➼ࡢᣲື

㸦() ್㸧ࡢᐃ⩏ࢆ♧ࡍࠋྛඖ⣲࡟ᑐࡍࡿ⃰⦰ಀᩘࡢ1-1 ඖ⣲⃰ᗘࡢᏘ⠇ኚື᭱኱್ࠊ᭱ᑠ್ࠊᖹᆒ್ࢆᅗ  ࡟♧ࡍࠋᅗ  ࡼࡾࠊ୰ᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡾࠊ2007 ᖺ 9 ᭶࠿ࡽ 2008࡯࡜ࢇ࡝ࡢඖ⣲ࡣ⮬↛Ⓨ⏕ⓗ࡞ࡶࡢ࡛࠶ࡿࡀ Znࠊᖺ 9 ᭶ࡲ࡛ࡢᕝᓮヨᩱ࠿ࡽ 27 ඖ⣲ NaࠊAlࠊScࠊSb ࡣ () ್ࡢᖹᆒ್ࡀࡑࢀࡒࢀ ࠊ ࡜  ௨ୖ࡛ࠊࣛࣥࢱࣀ࢖ࢻ➼ ࡀᐃ㔞ࡉࢀࡓࠋᐃ㔞ࡉࢀࡓᅵተ㉳※ேⅭⓎ⏕ⓗ࡜⪃࠼ࡽࢀࡿࠋ

ඖ⣲ AlࠊScࠊFeࠊLa ࡜ᾏὒ㉳※ඖ⣲ Na ࡢඖ⣲⃰EFx䋽(Cx/CAl)D/(Cx/CAl)R (1)ᗘ㸦ȣJJ㸧ࡢ᭶ูኚ໬ࢆᅗ  ࡟♧ࡍࠋᅗ  ࡼࡾࠊᅵCx :໧㗴䈫䈭䉎ర⚛Ớᐲተ㉳※ඖ⣲ࡣ᫓Ꮨ࡟ࣆ࣮ࢡࢆᣢࡕࠊᾏὒ㉳※ඖ⣲ࡣC䌁l䋺䌁䌬Ớᐲ᫓Ꮨ࡜ኟᏘ㹼⛅Ꮨ࡟ࣆ࣮ࢡࢆᣢࡗࡓࠋ୧㉳※ඖ⣲࡜ᷝሼ䌄䋺㒠ਅ‛ࡶ᫓Ꮨࡢࣆ࣮ࢡ࡟ࡘ࠸࡚ࡣࠊ೫す㢼ࡢᙳ㡪࡟ࡼࡾ࢔ᷝሼ䌒䋺࿾Ზሽ࿷ᐲ

ࢪ࢔኱㝣࠿ࡽ⢏Ꮚࡀ㣕᮶ࡋࡓࡓࡵࠊ࡯࠿ࡢ᭶ࡼࡾࡶ
ከ㔞࡟㝆ୗࡋࡓ࡜⪃࠼ࡽࢀࡿࠋᾏὒ㉳※ඖ⣲ Na ࡟ࡘ࠸࡚ࡣࠊࢺࣛࢪ࢙ࢡࢺ࣮ࣜࡢศᯒ⤖ᯝࡼࡾࠊኴᖹ
ὒഃ࠿ࡽࡢᾏሷ⢏Ꮚࡀཎᅉ࡛ኟᏘ㹼⛅Ꮨ࡟ࣆ࣮ࢡࢆ


㪈㪇㪇㪇

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ᣢࡗࡓ࡜⪃࠼ࡽࢀࡿࠋࡲࡓࠊ ᖺ  ᭶࡟ྎ㢼ࡀ 㪈㪇ᗘୖ㝣ࡋ࡚࠸ࡿࡓࡵࠊ ᖺ  ᭶ࡢ Na ࡢࣆ࣮ࢡࡣ

㪉㪌㪅㪇
㪉㪇㪅㪇
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㪪 㪺 㪃㪣㪸ర ⚛ Ớ ᐲ 䋨 㱘 㪾㪆 㪾䋩

㪐
㪏
㪎
㪍
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㪈
㪇

㪈

㪇㪅㪈
㪥㪸 㪪㪺 㪚㪸 㪚㫉 㪫㫀

㪥㪸
㪘㫃
㪪㪺
㪝㪼
㪣㪸

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㪭 㪤㫅 㪝㪼 㪱㫅 㪪㪹 㪣㪸 㪚㪼 㪜㫌 㪪㫄 㪛㫐 㪫㫄 㪟㪽 㪫㪿ᅗ 2 ⃰⦰ಀᩘ㸦2007 ᖺ 9 ᭶㹼2008 ᖺ 9 ᭶㸧⤫ィᏛⓗ୺ᡂศศᯒ࡟ࡼࡿ᳨ウ ୰ᛶᏊᨺᑕ໬ศᯒࡢ⤖ᯝࢆヲࡋࡃホ౯ࡍࡿࡓࡵ࡟㪉㪇㪇㪉 㪇 㪎ᐕ㪇㪎 㪐 ᦬㪉㪇 ᐕ 㪈㪇 㪎 㪇᦬㪉㪇 ᐕ 㪈㪇 㪎 㪈᦬ᐕ㪉㪇 㪈㪉㪇㪏 ᦬㪉 㪇 ᐕ㪈㪇㪏 ᦬㪉 㪇 ᐕ㪉㪇㪏 ᦬㪉 㪇 ᐕ㪊㪇㪏 ᦬㪉 㪇 ᐕ㪋㪇㪏 ᦬㪉 㪇 ᐕ㪌㪇㪏 ᦬㪉 㪇 ᐕ㪍㪇㪏 ᦬㪉 㪇 ᐕ㪎㪇㪏 ᦬㪉 㪇 ᐕ㪏㪇㪏 ᦬ᐕ㪐᦬㪥 㪸㪃㪘 㫃㪃㪝㪼 ర ⚛ Ớ ᐲ 䋨 䋦 䋩ྎ㢼ࡀ㉳ᅉࡋ࡚࠸ࡿྍ⬟ᛶࡀ࠶ࡿࠋ

⤫ィᏛⓗ࡞୺ᡂศศᯒࢆ⾜ࡗࡓࠋศᯒ࡟ࡣᾏὒ㉳※ඖ⣲ Naࠊᅵተ㉳※ඖ⣲ AlࠊThࠊScࠊFeࠊCeࠊLaࠊ    ᅗ 1 ඖ⣲⃰ᗘࡢ᭶ูኚ໬

ேⅭ㉳※ඖ⣲ ZnࠊSb ࡢඖ⣲⃰ᗘ㸦ȣJJ㸧ࠊẼ㇟ᅉᏊࠊ᭶㛫㝆ୗ㔞ࢆᅉᏊ࡟⏝࠸ࡓࠋ

1-2 ⃰⦰ಀᩘࢆ⏝࠸ࡓ㉳※ࡢ᳨ウ ⾲  ࡣ୺ᡂศศᯒࡢ⤖ᯝ࡛࠶ࡿࠋ➨  ୺ᡂศ࡟ᑐ

୰ᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡾᐃ㔞ࡉࢀࡓඖ⣲ࡀ⮬↛Ⓨࡋ࡚ࡣᅵተ㉳※ඖ⣲ࡀᙉ࠸ᅉᏊ㈇Ⲵ㔞ࢆᣢࡗ࡚࠸ࡿࠋ

3-11- 357 -

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JAEA-Review 2013-039

ࡲࡓẼ㇟ᅉᏊࡀᅉᏊ㈇Ⲵ㔞ࢆᣢࡓ࡞࠸ࡇ࡜ࢆ⪃៖ࡍ

1-4 Ca ࡜ࢺࣛࢪ࢙ࢡࢺ࣮ࣜࢆ⏝࠸ࡓ㯤◁ࡢ㣕᮶ࡿ࡜ࠊ➨㸯୺ᡂศࡣࠊᅵተ㉳※ඖ⣲ࡀ⮬⏤ⴠୗ࡟ࡼ୰ᛶᏊᨺᑕ໬ศᯒ࡛ᐃ㔞ࡉࢀࡓ Ca ⃰ᗘ㸦㸣㸧࡜ࡾ㝆ୗࡍࡿࡇ࡜ࢆ♧ࡋ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋ➨  ୺ࢺࣛࢪ࢙ࢡࢺ࣮ࣜࡢศᯒ⤖ᯝࢆ⏝࠸࡚㯤◁ࡢ㝆ୗ⌧ᡂศ࡟ᑐࡋ࡚ࡣࠊZn ࡜ Sb ࡀᙉ࠸ᅉᏊ㈇Ⲵ㔞ࢆᣢࡗ㇟ࡢ᭶ูኚ໬࡟ࡘ࠸᳨࡚ウࡋࡓࠋᅗ  ࡣ Ca ⃰ᗘࡢ࡚࠸ࡿࡇ࡜࠿ࡽࠊ➨  ୺ᡂศࡣ Zn ࡜ Sb ࡢ┦㛵㛵ಀ᭶ูኚ໬ࢆ♧ࡋࡓࢢࣛࣇ࡛࠶ࡿࠋᅗ  ࡼࡾࠊCa ⃰ᗘࢆ♧ࡋ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋ➨  ୺ᡂศ࡛ࡣᾏὒ㉳ࡣ෤Ꮨ࠿ࡽ᫓ඛ࡟࠿ࡅ࡚㧗࠸್ࢆ♧ࡍࡇ࡜ࡀࢃ࠿ࡿࠋ

※ඖ⣲ Naࠊ᭶㛫㝆Ỉ㔞ཬࡧ᭶㛫ᖹᆒẼࡀᙉ࠸ᅉࢺࣛࢪ࢙ࢡࢺ࣮ࣜࡢศᯒ⤖ᯝࡼࡾ෤Ꮨ࠿ࡽ᫓ඛࡣ࢔

Ꮚ㈇Ⲵ㔞ࢆᣢࡗ࡚࠸ࡿࡇ࡜࠿ࡽࠊ➨  ୺ᡂศ࡛ࡣᾏ

ࢪ࢔኱㝣࠿ࡽ⢏Ꮚࡀ㣕᮶ࡋ࡚࠸ࡿࡇ࡜ࡀࢃ࠿ࡗࡓࠋ

ሷ⢏Ꮚ࡟ྵࡲࢀ࡚࠸ࡿ Na ࡀ᭶㛫㝆Ỉ㔞࡜┦㛵ࢆᣢCa ࡣ㯤◁࡟ྵࡲࢀࡿ୺࡞ඖ⣲ࡢࡦ࡜ࡘ࡞ࡢ࡛ࠊᑡ࡞

ࡘࡇ࡜ࢆ♧ࡋ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋ

ࡃ࡜ࡶ᫓Ꮨࡣ࢔ࢪ࢔኱㝣࠿ࡽ೫す㢼࡟஌ࡗ࡚㯤◁ࡀḟ࡟ࠊ➨  ୺ᡂศࡢ⤖ᯝ࠿ࡽᾏὒ㉳※ඖ⣲ Na ࡜

㣕᮶ࡍࡿ࡜⪃࠼ࡽࢀࡿࠋ

Zn ࡀ┦㛵㛵ಀ࡟࠶ࡿྍ⬟ᛶࡀ♧၀ࡉࢀࡓࡢ࡛ࠊNaࠊ
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㹼 ᭶ࡢᾏὒ㉳※ඖ⣲࡜ேⅭ㉳※ඖ⣲ࡢ⃰ᗘࡢ┦㛵ಀᩘ࡛࠶ࡿࠋࡇࢀࡼࡾࠊኟᏘ࡟࠾࠸࡚ྛඖ⣲⃰ᗘࡀࡑࢀࡒࢀࡢඖ⣲⃰ᗘ࡟ᑐࡋ࡚㧗࠸ṇࡢ┦㛵ࢆ♧ࡋ࡚ర ⚛ Ớ ᐲ 䋨䋦 䋩

Zn ཬࡧ Sb ࡢ┦㛵ಀᩘࢆ⟬ฟࡋࡓࠋ⾲  ࡣ  ᖺ 

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ᐕ
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㪇㪎 ᦬
ᐕ
㪉㪇 㪈㪈
㪇㪎 ᦬
ᐕ
㪉 㪇 㪈 㪉᦬㪇㪏ᐕ㪉 㪇 㪈᦬㪇㪏ᐕ㪉 㪇 㪉᦬㪇㪏ᐕ㪉 㪇 㪊᦬㪇㪏ᐕ㪉 㪇 㪋᦬㪇㪏ᐕ㪉 㪇 㪌᦬㪇㪏ᐕ㪉 㪇 㪍᦬㪇㪏ᐕ㪉 㪇 㪎᦬㪇㪏ᐕ㪉 㪇 㪏᦬㪇㪏ᐕ㪐᦬࠸ࡿࡇ࡜ࡀࢃ࠿ࡿࠋ ࡢ᳨ウ࠿ࡽࠊNa ࡣኟᏘ࡟࠾
࠸࡚ኴᖹὒഃ࠿ࡽ㣕᮶ࡍࡿ࡜⪃࠼ࡽࢀࡿࡢ࡛ࠊ┦㛵ಀᩘ࠿ࡽ ZnࠊSb ࡶኴᖹὒഃ࠿ࡽ㣕᮶ࡍࡿ࡜⪃࠼ࡽ

ᅗ 3 Ca ⃰ᗘࡢ᭶ูኚ໬

ࢀࡿࠋࡲࡓࠊZn ࡟ࡘ࠸࡚ࡣᗫᲠ≀ࡢ⇞↝ࡲࡓࡣ⮬ື㌴ࡢ᤼࢞ࢫࠊSb ࡟ࡘ࠸࡚ࡣᗫᲠ≀ࡢ⇞↝ࡲࡓࡣ⮬ື㌴ࡢࢱ࢖ࣖࡢᦶ⪖࡟ࡼࡾ᤼ฟࡉࢀࡿࠋ᥇ྲྀᆅⅬࡢ༡ᮾ⣙ .P ࡟ࡣᮾྡ㧗㏿㐨㊰ࡸᅜ㐨  ྕࡀ࠶ࡿࡢ࡛ࠊ
⮬ື㌴ࡀ ZnࠊSb ࡢ᤼ฟ※࡟࡞ࡗ࡚࠸ࡿྍ⬟ᛶࡀ࠶ࡿࠋࡋ࠿ࡋࠊZnࠊSb ࡣᗫᲠ≀ࡢ⇞↝࠿ࡽࡶ᤼ฟࡉ
ࢀࡿࡢ࡛ࠊࡇࢀࡽࡢඖ⣲ࡢ㉳※ࡣูࠎࡢྍ⬟ᛶࡶ࠶
ࡿࠋ

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2㸬኱Ẽ⢏Ꮚ≧≀࡟࠾ࡅࡿᚤ㔞ඖ⣲➼ࡢᣲື
2-1 210Pbᨺᑕ⬟࡜7Beᨺᑕ⬟ࡲࡎAPM⃰ᗘ࡜210Pbᨺᑕ⬟⃰ᗘࡢ㛵ಀࢆㄪ࡭ࡿࡓࡵ࡟ࠊAPM⃰ᗘ࡜210Pbᨺᑕ⬟⃰ᗘࡢ┦㛵ಀᩘࢆồࡵࡓ࡜ࡇࢁ┦㛵ಀᩘࡣR㸻0.69 ࡛࠶ࡗࡓࠋࡲࡓࠊ
㢼㏿࡜㝆Ỉ㔞࡛つ᱁໬ࡋࡓ࡜ࡇࢁࠊ┦㛵ಀᩘࡣࡑࢀ
ࡒࢀR=0.80ࠊR=0.98 ࡜࡞ࡾࠊ㝆Ỉ㔞࡛つ᱁໬ࡋࡓሙྜࡣ㠀ᖖ࡟ᙉ࠸┦㛵ࢆ♧ࡋࡓࠋᅗ 4 ࡟㝆Ỉ㔞࡛つ

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㒠᳓㊂
᳇᷷
㒠ਅ‛㊂

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㪄 㪇 㪅㪇 㪉㪇 㪅㪈 㪍㪇 㪅㪊 㪇㪄 㪇 㪅㪉 㪋㪄 㪇 㪅㪍 㪌㪄 㪇 㪅㪇 㪎╙㪊╙㪋㪇 㪅㪌 㪎㪄 㪇 㪅㪇 㪌㪇 㪅㪉 㪌㪄 㪇 㪅㪉 㪊㪇 㪅㪇 㪌㪇 㪅㪊 㪉㪇 㪅㪊 㪋㪄 㪇 㪅㪇 㪌㪇 㪅㪊 㪎㪇 㪅㪇 㪏㪇 㪅㪏 㪌㪇 㪅㪌 㪊㪇 㪅㪇 㪈㪄 㪇 㪅㪊 㪎㪄 㪇 㪅㪊 㪎㪄 㪇 㪅㪇 㪋㪄 㪇 㪅㪉 㪈㪇 㪅㪉 㪇㪇 㪅㪇 㪇㪇 㪅㪉 㪇㪇 㪅㪎 㪍㪇 㪅㪏 㪍㪄 㪇 㪅㪎 㪍㪄 㪇 㪅㪇 㪊㪄 㪇 㪅㪉 㪈㪄 㪇 㪅㪐 㪋㪇 㪅㪍 㪉㪄 㪇 㪅㪉 㪍㪇 㪅㪈 㪐㪄 㪇 㪅㪇 㪌㪄 㪇 㪅㪉 㪈㪄 㪇 㪅㪇 㪉㪇 㪅㪇 㪏㪇 㪅㪌 㪏㪇 㪅㪇 㪏㪇 㪅㪉 㪐㪄 㪇 㪅㪉 㪐㪄 㪇 㪅㪋 㪈㪇 㪅㪉 㪋

᱁໬ࡋࡓሙྜࡢAPM⃰ᗘ࡜210Pbᨺᑕ⬟⃰ᗘࢆ♧ࡍࠋ
࡞࠾7Be࡟ࡘ࠸࡚ࡶྠᵝࡢഴྥࢆ♧ࡋࡓࠋ㪇㪅㪇㪋㪌㒠᳓㊂䈅䈢䉍䈱210Pb᡼኿⢻[mBq/m3/㷔]⾲ 2 ୺ᡂศศᯒ
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⾲ 3 ┦㛵ಀᩘ

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PMỚᐲ[mg/m3 /㷔]ᅗ 4 㝆Ỉ㔞࠶ࡓࡾࡢAPM⃰ᗘ࡜210Pbᨺᑕ⬟

3-11- 358 -

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JAEA-Review 2013-039⥆࠸࡚㢼ྥ࡜ࡢ㛵ಀ࡟╔┠ࡋ࡚ࡳࡿ࡜ࠊ໭㢼ࡀ྿࠸㒠᳓㊂䈅䈢䉍䈱210Pb᡼኿⢻[mBq/m3/㷔]㪊㪅㪇ࡓ᫬ࡣ༡㢼ࡀ྿࠸ࡓ᫬࡜ẚ㍑ࡋ࡚ࠊᨺᑕ⬟⃰ᗘࡀ⣙㪉㪅㪌

1.3 ಸ㧗࠸್ࢆ♧ࡋࡓࠋࡑࡢࡓࡵࠊ༡㢼ࡀ྿ࡃ 6 ᭶㪉㪅㪇࠿ࡽ 8 ᭶࡟࠿ࡅ࡚ࠊᨺᑕ⬟⃰ᗘࡀపࡃ࡞ࡿᏘ⠇ኚື

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ࢆ♧ࡍࡇ࡜ࡀศ࠿ࡗࡓࠋࡇࡢࡇ࡜ࡣࠊ210Pbࡢ㉳※ࡀ⑺୺࡟኱㝣ࡢᅵተ࡛࠶ࡿࡇ࡜ࠊࡲࡓ7Beࡢ㉳※ࡀ୺࡟

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㧗⦋ᗘᆅᇦ࡛࠶ࡿࡇ࡜࡟㉳ᅉࡋ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋ

㪍㒠᳓㊂䈅䈢䉍䈱 7 Be᡼኿⢻ [mBq/m3 /㷔]ࡇࡢࡇ࡜ࡣᅗ 7 ࡟♧ࡋࡓ 2008 ᖺࡢ෤(1 ᭶㹼2 ᭶)࡜

ᅗ 5 㝆Ỉ㔞࠶ࡓࡾࡢ210Pb࡜7Beࡢ㛵ಀኟ(6 ᭶㹼8 ᭶)ࡢࢺࣛࢪ࢙ࢡࢺ࣮ࣜศᯒࡢ⤖ᯝ࠿ࡽࡶḟ࡟210Pb࡜7Be୧᰾✀ࡢ㛵ಀࢆㄪ࡭ࡿࡓࡵ࡟ࠊྠ

⿬௜ࡅࡽࢀ࡚࠸ࡿࠋ

ᵝ࡟┦㛵ಀᩘࢆồࡵࡓ࡜ࡇࢁR=0.84 ࡜ᙉ࠸┦㛵ࢆ࡟ࠊ㢼㏿࡜㝆Ỉ㔞࡛つ᱁໬ࡋࡓୖ࡛┦㛵ಀᩘࢆồࡵࡿ࡜ࠊࡑࢀࡒࢀR=0.95ࠊR=0.99 ࡜࡞ࡾ㠀ᖖ࡟ᙉ࠸┦㛵ࢆ♧ࡋࡓࠋࡇࡢࡇ࡜࠿ࡽAPM⃰ᗘࠊ210Pbཬࡧ
7Beᨺᑕ⬟⃰ᗘࡣ㝆Ỉ⌧㇟࡜㢼㏿࡟ᨭ㓄ࡉࢀ࡚࠸ࡿ

㪊㪌᦬㑆䈱 210Pb᡼኿ ⢻ [Bq/㷔 ]♧ࡋࡓࠋࡉࡽ࡟APM⃰ᗘ࡜ᨺᑕ⬟⃰ᗘࡢ㛵ಀ࡜ྠᵝ

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ࡇ࡜ࡀศ࠿ࡿࠋᅗ 5 ࡟㝆Ỉ㔞࠶ࡓࡾࡢ210Pbᨺᑕ⬟⃰㪌ᗘ࡜7Beᨺᑕ⬟⃰ᗘࢆᏘ⠇ู࡟♧ࡍࠋ

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᦬㑆㒠᳓㊂[mm]ᅗ 6 210PbࡢᏘ⠇ኚື

2-2 Ꮨ⠇ኚື
210Pb࡜7BeࡢᏘ⠇ኚືࢆㄪ࡭ࡿࡓࡵ࡟ࠊ┦㛵㛵ಀࡢ࠶ࡿ㝆Ỉ⌧㇟࡜㢼࡜ࡢ㛵ಀࢆ฼⏝ࡍࡿࠋࡲࡎ㝆Ỉ⌧㇟࡟ࡼࡿᏘ⠇ኚືࢆㄪ࡭ࡿࡓࡵ࡟ࠊᅗ 6 ࡟᭶㛫ࡢ㝆Ỉ㔞࠶ࡓࡾࡢ210Pbᨺᑕ⬟࡜㝆Ỉ㔞ࡢ㛵ಀࢆ♧ࡍࠋ
ᅗ 6 ࡼࡾࠊᨺᑕ⬟ࡣ෤࡟㧗ࡃ࡞ࡾࠊࡑࡢ௚ࡢᏘ⠇࡛పࡃ࡞ࡿഴྥࢆ♧ࡋࡓࠋࡇࢀࡣᱵ㞵ࡢ᫬ᮇࡸࠊኟ࠿
ࡽ⛅࡟࠿ࡅ࡚᪥ᮏ࡟᥋㏆ࡋ࡚ࡃࡿྎ㢼ࡀ㞵ࢆ኱㔞࡟ࡶࡓࡽࡍࡇ࡜࡟ࡼࡗ࡚wash-outຠᯝࡀ㉳ࡇࡾࠊ

ᅗ 7 2008 ᖺ෤࡜ኟࡢࢺࣛࢪ࢙ࢡࢺ࣮ࣜ

APM⃰ᗘࡀపࡃ࡞ࡗࡓࡇ࡜࡟㉳ᅉࡋ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋࡲࡓᅗ 6 ࡟࠾࠸࡚ࠊኟ࡟㧗࠸್ࢆ♧ࡋ࡚࠸ࡿ⟠ᡤࡀ࠶ࡿࡀࠊࡇࢀࡣ㸵᭶ࡢࢹ࣮ࢱ࡛࠶ࡿࠋ2008

2-3 ᨺᑕ໬ศᯒࡢᐃ㔞⤖ᯝ࡜Ⓨ⏕㉳※ᖺ 7 ᭶ࡣ౛ᖺ࡜ẚ㍑ࡋ࡚㝆Ỉ㔞ࡀ኱ᖜ࡟ᑡ࡞࠿ࡗࡓ

2003 ᖺ 7 ᭶࠿ࡽ 9 ᭶ࡢ 13 ᮇ㛫࡟࠾ࡅࡿ APM ࡟ࡓࡵࠊ෤ࡢ᫬ᮇ࡜ఝࡓഴྥࢆ♧ࡋࡓࠋᚑࡗ࡚210Pbᨺ࠾࠸࡚ 19 ✀㢮ࡢඖ⣲ࠊ2007 ᖺཬࡧ 2008 ᖺࡢ 7 ᭶ᑕ⬟ࡢᏘ⠇ኚືࡣ㝆Ỉ⌧㇟࡜ᐦ᥋࡟㛵ಀࡋ࡚࠾ࡾࠊ

࠿ࡽ 9 ᭶ࡢ 13 ᮇ㛫࡟࠾࠸࡚ࡣ 26 ✀㢮ࡢඖ⣲ࡀᐃ㔞

APM࡜㝆Ỉ⌧㇟ࡢᐦ᥋࡞㛵ಀࢆ⿬௜ࡅ࡚࠸ࡿࠋ࡞࠾

࡛ࡁࡓࠋ

7Be࡟ࡘ࠸࡚ࡶྠᵝࡢഴྥࢆ♧ࡋࡓࠋᐃ㔞࡛ࡁࡓඖ⣲ࡢⓎ⏕㉳※ࢆ᥎ᐹࡍࡿࡓࡵ࡟⃰⦰ḟ࡟㢼࡜ࡢ㛵ಀ࠿ࡽᏘ⠇ኚືࢆㄪ࡭ࡿࠋࡲࡎᖹᆒಀᩘ(Enrichment Factor, E.F.)ࢆồࡵࡓࠋE.F.್ࡣ

㢼㏿࡟ࡘ࠸࡚ࡣࠊ኱ࡁ࡞Ꮨ⠇ኚືࢆ♧ࡉࡎࠊ210Pb࡜

௨ୗࡢᘧ࡛ᐃ⩏ࡉࢀࠊࡇࡢ್ࡀ 1 ࡟㏆࠸࡯࡝⮬↛㉳

7Be࡜ࡢ㛵ಀ࡟࠾࠸࡚ࡶᏘ⠇ኚືࡣぢฟࡏ࡞࠿ࡗࡓࠋ

※ࡢᐤ୚ࡀ኱ࡁ࠸ࡇ࡜ࢆព࿡ࡍࡿࠋ

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JAEA-Review 2013-039

E .F .

>X Al @APMࡣ┦㛵ࢆ♧ࡉ࡞࠿ࡗࡓࠋࡑࡢࡓࡵ Zn ࡜ Cl ࡣ௚ࡢ㉳

>X Al @ᆅẆ※ࡢᙳ㡪ࡀ኱ࡁࡃࠊ࢞ࢯࣜࣥࡢῧຍ๣࡜ࡋ࡚⏝࠸ࡽ

X㸸ὀ┠ࡍࡿඖ⣲⃰ᗘࢀࡿ Br ࡀ⮬ື㌴㉳※ࡢඖ⣲ࡔ࡜⪃࠼ࡽࢀࡿࠋࢧࣥ

Al㸸Al ࡢඖ⣲⃰ᗘࣉࣜࣥࢢᆅⅬࡢ༡ᮾ⣙ 3km ࡟㧗㏿㐨㊰ࡸᖿ⥺㐨㊰

E.F.್ࢆồࡵࡓ⤖ᯝࢆᅗ 8 ࡟♧ࡍࠋᅗ 8 ࡼࡾࠊᖹࡀ㏻ࡗ࡚࠸ࡿࡓࡵࠊࡇࡇ࠿ࡽࡢᙳ㡪ࢆཷࡅ࡚࠸ࡿྍ

ᆒ್࠿ࡽࡢࡎࢀ➼ࢆ⪃៖ࡋ࡚ E.F.್ 10 ᮍ‶ࢆ⮬↛⬟ᛶࡀ࠶ࡿࠋ㕲㗰ᴗ࣭㠀㕲㔠ᒓ㖔ᴗ㉳※ࡢඖ⣲ࡣ Cr,㉳※ඖ⣲ࠊ10 ௨ୖࢆேⅭ㉳※ඖ⣲࡜ࡋࡓࠋMn, Fe, Cu, Zn, As, Sm ࡀᣲࡆࡽࢀࡿࠋࡇࢀࡽࡢඖ

ࡲࡓඖ⣲㛫ࡢ㛵ಀࢆㄪ࡭ࡿࡓࡵ࡟ࠊྛඖ⣲㛫ཬࡧ⣲ࡣࢧࣥࣉࣜࣥࢢᆅⅬ༡ᮾࡢᕤᴗᆅᖏ࠿ࡽࡢ᤼ฟࡀ
⪃࠼ࡽࢀࡿࡀࠊ┦஫ࡢ┦㛵ࡀᙅ࠸ࡓࡵᙳ㡪ࡣ㠀ᖖ࡟ྛඖ⣲࡜Ẽ㇟ᅉᏊࡢ┦㛵ಀᩘࢆồࡵࡓࠋࡲࡎ⮬↛㉳※ࡢඖ⣲࡟ࡘ࠸࡚ࡣࠊⓎ⏕㉳※ࢆᅵተᑠࡉ࠸ࡶࡢ࡜⪃࠼ࡽࢀࡿࠋ⫧ᩱ㉳※ࡢඖ⣲࡟ࡣ U ࡀ࡜ᾏሷ࡟ศࡅࡿࡇ࡜ࡀ࡛ࡁࡿࠋᅵተ㉳※ඖ⣲ࡣ Al,

࠶ࡿࠋE.F.್࠿ࡽ U ࡣேⅭ㉳※ඖ⣲࡛࠶ࡿࡢ࡛ࠊ⏿Sc, Ti ࡸࣛࣥࢱࣀ࢖ࢻ➼ࡀᣲࡆࡽࢀࠊAl, Sc, Ti ࡀ┦࡞࡝࡬ࡢ᪋⫧ࡢᙳ㡪ࢆཷࡅࡓ࡜⪃࠼ࡽࢀࡿࠋ

஫࡟ᙉ࠸┦㛵(R=0.82㹼0.90)ࢆ♧ࡋࠊࣛࣥࢱࣀ࢖ࢻ

1.0E+04࡜ࡶ┦㛵(R=0.35㹼0.61)ࢆ♧ࡋࡓࠋࡲࡓࠊࡇࢀࡽࡢ
ඖ⣲࡜ Ca, Cr, Mn, Fe, Zn ࡀẚ㍑ⓗᙉ࠸┦㛵
1.0E+03(R=0.55㹼0.81)ࢆ♧ࡋࡓࡇ࡜࠿ࡽࠊCa, Cr, Mn, Fe,
Zn ࡶᅵተ㉳※ࡢᙳ㡪ࢆཷࡅ࡚࠸ࡿඖ⣲࡜ゝ࠼ࡿࠋᾏ
1.0E+02

䌅.䌆 .୯

ሷ㉳※ඖ⣲ࡣ Na, Cl, Ca, Br ࡀᣲࡆࡽࢀࡿࠋNa ࡣ༡㢼ࡢ㢼㏿࡜ẚ㍑ⓗᙉ࠸┦㛵(R=0.73)ࢆ♧ࡋࡓࡇ࡜

1.0E+01࠿ࡽᾏሷ㉳※࡛࠶ࡿ࡜ゝ࠼ࠊNa ࡜ẚ㍑ⓗᙉ࠸┦㛵(R=0.63)ࢆ♧ࡋࡓ Cl ࡶᾏሷ㉳※ࡔ࡜⪃࠼ࡽࢀࡿࠋ
Ca ࡜ Br ࡣ Na ࡸ Cl ࡜ࡣ┦㛵ࢆ♧ࡉ࡞࠿ࡗࡓࡇ࡜

1.0E+00

࠿ࡽࠊCa ࡣᅵተࠊBr ࡣேⅭ㉳※࠿ࡽࡢᙳ㡪ࡀ኱ࡁ࠸࡜⪃࠼ࡽࢀࡿࠋ

Al
Ti
Fe
Sc
Mn
Ca
Sm
Eu
V
La
Ce
Th
Dy
Mg
Na
Cr
Hf
U
Cu
Tm
Zn
As
Br
Mo
Sb

1.0EͲ01ర⚛ฬḟ࡟ேⅭ㉳※ࡢඖ⣲࡟ࡘ࠸࡚ࡣࠊⓎ⏕㉳※ࢆ୺࡟ᅗ8▼Ἔ⇞↝⣔⢏ᏊࠊᗫᲠ≀↝༷⣔⢏Ꮚࠊ⮬ື㌴ࠊ㕲㗰ࠊ㠀㕲㔠ᒓ㖔ᴗࠊ⫧ᩱ࡟ศࡅࡿࡇ࡜ࡀ࡛ࡁࡿࠋ▼Ἔ⇞↝⣔⢏Ꮚ㉳※ࡢඖ⣲ࡣࠊMg, V, Mn, Fe,Cu, Zn, As࡞࡝ࡀᣲࡆࡽࢀࡿࠋࡇࡢ୰࡛ E.F.್࠿ࡽேⅭ㉳※࡟ศ㢮ࡉࢀࡓࡢࡣ Cu, Zn, As ࡛࠶ࡾࠊࡇࢀࡽࡣ┦஫࡟[ᡂᯝࡢබ⾲]Ϩ㸬Ꮫ⾡ㄅ
㸯㸬M. Suzuki and T. Honda㸹Investigation of theorigin and sedimentary environment of marine┦㛵(R=0.49㹼0.56)ࢆ♧ࡋࡓࠋࡲࡓ Mn, Fe ࡣ Zn

sediments from coastal areas of western Japan࡜┦㛵(ࡑࢀࡒࢀ R=0.74, R=0.70)ࢆ♧ࡋࡇ࡜࠿ࡽࠊ

by INAA, Journal of Radioanalytical andᑡ࡞࠿ࡽࡎᙳ㡪ࢆ୚࠼࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋᗫᲠ≀Nuclear↝༷⣔⢏Ꮚ㉳※ࡢඖ⣲ࡣ Zn, Sb ࡀᣲࡆࡽࢀࠊZn ࡜
Sb ࡢ┦㛵ࢆㄪ࡭ࡿ࡜ࠊẚ㍑ⓗᙉ࠸┦㛵(R=0.75)ࢆ♧ࡋࡓࠋࡲࡓ㢼㏿࡜ࡢ┦㛵ࢆㄪ࡭ࡓ࡜ࡇࢁࠊ༡㢼࡟ᑐ⃰⦰ಀᩘ(2003ࠊ2007 ཬࡧ 2008 ᖺࡢ 7 ᭶࠿ࡽ 9 ᭶㸧Chemistry,

vol.278(No.2),

337-341(2008)
㸰㸬K. Oda, Y. Kikawada, T. Oi and T. Honda㸹ࡋ࡚㈇ࡢ┦㛵ࢆ♧ࡋࡓࡇ࡜࠿ࡽࢧࣥࣉࣜࣥࢢᆅⅬࡢ໭ഃ࠿ࡽࡢ㐠ࡤࢀ࡚ࡁࡓྍ⬟ᛶࡀ㧗࠸ࠋ⮬ື㌴㉳※
ࡢඖ⣲ࡣ Zn, Cl, Br ࡀᣲࡆࡽࢀࡿࡀࠊࡇࢀࡽࡢඖ⣲- 360 -

Behaviorsofchemicalelements

intheatmosphere, Kawasaki, Japan, Journal ofRadioanalytical and Nuclear Chemistry, vol.278

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JAEA-Review 2013-039

11㸬T. Honda and Y. Satoh㸹Sedimentary(No.2), 475-478(2008)
㸱㸬T. Honda and H. Pettersson㸹Determination ofenvironment in marine sediments from twolanthanoids and uranium in groundwater fromcoastal areas in the Kyushu district, Bull.

southeast

Atomic Energy Research laboratory, Musashi

Swedenbyneutronactivation

analysis and their behavior including uranium
seriesnuclides,RADIOISOTOPES,

Institute of Technology, No. 33, 7-15(2007)12㸬᪩ὠᓅᏹ㸪ᮌᕝ⏣႐୍㸪ᮏከ↷ᖾ㸪኱஭㝯ኵ㸹

vol.57(No.1), 71-78 (2008)ⅆᒣᛶᾏᗏሁ✚≀ࡢᚤ㔞ඖ⣲ᙧែูศᯒ࡟࠾ࡅࡿ

㸲 㸬 T. Honda and Y. Satoh 㸹 Sedimentary㏲ḟ⁐ゎἲࡢ㐺⏝㸪Ṋⶶᕤᴗ኱ᏛཎᏊຊ◊✲ᡤ

environment and origin of marine sedimentsሗ㸪㏻ᕳ 33 ྕ㸪16-28(2007㸧

collected from Kagoshima Bay and Shimabara

13㸬ᮏከ↷ᖾ㸪ᚋ⸨ோ⨾㸪໭ཎ↷ኸ㸹2003-2004 ᖺ

Bay in Kyushu, Japan, Bulletin of the Society ofᕝᓮ኱Ẽ⎔ቃ୰ࡢ210Pb࠾ࡼࡧ7BeࡢᏑᅾ㔞࡜ᣲ

Sea Water Science, Japan, vol.62 (No.1),ື㸪ࣇ࢕ࢵࢩ࣭ࣙࣥࢺࣛࢵࢡ ࢽ࣮ࣗࢫࣞࢱ࣮㸪

28-34(2008)➨ 19 ྕ㸪27-31(2006)5㸬ᮌᕝ⏣႐୍㸪ᑠ⏣ᖾᖹ㸪ᮏከ↷ᖾ㸪኱஭㝯ኵ㸹

14㸬㕥ᮌ⨾ဏ㸪ᮏከ↷ᖾ㸹ఀໃ‴୪ࡧ࡟኱㜰‴ᾏᗏᨺᑕᛶ㝆ୗ≀ᶆ‽ヨᩱࡢ࢘ࣛࣥྠ఩యẚ㸪Ṋሁ✚≀୰ࡢ࢘ࣛࣥ㸪ࢺ࣒ࣜ࢘ཬࡧࣛࣥࢱࣀ࢖ࢻࡢ

ⶶᕤᴗ኱ᏛཎᏊຊ◊✲ᡤሗ㸪㏻ᕳ 34 ྕ㸪ศᕸ࡜ᣲື㸪ࣇ࢕ࢵࢩ࣭ࣙࣥࢺࣛࢵࢡ ࢽ࣮ࣗࢫ21-27(2008)ࣞࢱ࣮㸪➨ 19 ྕ㸪33-37(2006)

㸴㸬す⏣▱ᗈ㸪ᮌᕝ⏣႐୍㸪ᮏከ↷ᖾ㸪኱஭㝯ኵ㸹⚄ዉᕝ┴ᮾ㒊ࡢ኱Ẽ⢏Ꮚ≧≀㉁࡟ྵࡲࢀࡿ஧ḟϩ㸬ཱྀ㢌Ⓨ⾲

⢏Ꮚࡢືែゎᯒ㸪Ṋⶶᕤᴗ኱ᏛཎᏊຊ◊✲ᡤሗ㸪

㸯㸬Y. Kikawada, K. Oda, T. Oi, M. Nomura, T.

㏻ᕳ 34 ྕ㸪28-39(2008)

Honda and K. Hirose; Uranium isotope ratios in㸵㸬ᔢᓚᾈᏊ㸪ᮏከ↷ᖾ㸹210Pb୪ࡧ࡟137Csࢆ⏝࠸

atmospheric deposits in Japan, 18th Annual V.

ࡓᮾி‴ᾏᗏሁ✚≀ࡢሁ✚ᖺ௦࡜࢖ࣥ࣋ࣥࢺ࣮ࣜ㸪M.

Goldschmidt

Conference,

Geochim.

ࣇ࢕ࢵࢩ࣭ࣙࣥࢺࣛࢵࢡ ࢽ࣮ࣗࢫࣞࢱ࣮㸪➨ 21

Cosmochim. Acta, 72, Suppl. 1, A469, 2008㸰㸬ᮌᕝ⏣႐୍㸪ᑠ⏣ᖾᖹ㸪኱஭㝯ኵ㸪㔝ᮧ㞞ኵ㸪ྕ㸪28-30(2008)㸶㸬Ọ⏣ᐶ㸪ᮏከ↷ᖾ㸪ᒾ᭶㍤ᕼ㸪Ỉ㔝ᓫ㸹ᮾ⃰࢘ᮏከ↷ᖾ㸪ᘅ℩຾ᕭ㸹ᅜෆ኱Ẽ㝆ୗ≀ヨᩱࡢ␗ᖖࣛࣥ㖔ᗋ࿘㎶ࡢ⍞ᾉᒙ⩌࡟⏘ࡍࡿሁ✚ᒾ㢮୰ࡢ࢘࢘ࣛࣥྠ఩యẚ㸪2008 ᖺᗘ᪥ᮏᆅ⌫໬Ꮫ఍➨ 55ࣛࣥ㸪ࢺ࣒ࣜ࢘ཬࡧࣛࣥࢱࣀ࢖ࢻࡢศᕸ࡜ᣲື㸪

ᅇᖺ఍ㅮ₇せ᪨㞟㸪p.345㸪2008ࣇ࢕ࢵࢩ࣭ࣙࣥࢺࣛࢵࢡ ࢽ࣮ࣗࢫࣞࢱ࣮㸪➨ 20㸱㸬Ọ⏣ᐶ㸪ᮏከ↷ᖾ㸪ᒾ᭶㍤ᕼ㸪Ỉ㔝ᓫ㸹ᆅ⌫໬Ꮫⓗ⎔ቃࡢ┦㐪࡟㉳ᅉࡍࡿሁ✚ᒾ୰ࡢᚤ㔞࣭୺せྕ㸪30-33(2007)ඖ⣲ࡢศᕸ࡜ᣲື㸪➨ 45 ᅇ࢔࢖ࢯࢺ࣮ࣉ࣭ᨺᑕ

㸷㸬ᮌᕝ⏣႐୍㸪᪩ὠᓅᏹ㸪๓ᕝ⿱Ꮚ㸪ᮏከ↷ᖾ㸪

⥺◊✲Ⓨ⾲఍せ᪨㞟㸪p.19㸪2008኱஭㝯ኵ㸹㏲ḟ⁐ゎἲࢆ⏝࠸ࡓⅆᒣᛶᾏᗏሁ✚≀ࡢᚤ㔞ඖ⣲ᙧែูศᯒ㸪᪥ᮏᾏỈᏛ఍ㄅ㸪➨ 61

㸲㸬M. Suzuki and T. Honda; Distribution andᕳ㸦➨ 5 ྕ㸧
㸪286-292(2007)

behavior of trace elements in marine sediments

10㸬M. Suzuki and T. Honda㸹Distribution andfrom coastal areas of western Japan, 12th

behavior of trace elements in marine sediments

International Conference on Modern Trends infrom coastal areas of western Japan, Bull.

Activation Analysis, pp. 92, 2007

Atomic Energy Research laboratory, Musashi

㸳㸬K. Oda, Y. Kikawada, T. Oi, and T. Honda;
Behavior of antimony in the atmosphere,

Institute of Technology, No. 34, 7-13(2007)

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JAEA-Review 2013-039

Kawasaki,Japan,

12th

International㸶㸬ᑠ⏣ᖾᖹ㸪ᮌᕝ⏣႐୍㸪኱஭㝯ኵ㸪ᮏከ↷ᖾ㸪

Conference on Modern Trends in Activationᘅ℩຾ᕭ㸹⚟ᒸ࡟࠾ࡅࡿ኱Ẽ㝆ୗ≀୰ࡢ࢘ࣛࣥྠ

Analysis, pp. 104, 2007఩యẚศᯒ㸪2007 ᖺᗘ᪥ᮏᆅ⌫໬Ꮫ఍➨ 54 ᅇᖺ
఍ㅮ₇せ᪨㞟㸪p.247㸪2007㸴㸬㕥ᮌ⨾ဏ㸪ᮏከ↷ᖾ㸹⣖ఀỈ㐨㸪ᗈᓥ‴ཬࡧᅵ
బ‴ᾏᗏሁ✚≀࡟࠾ࡅࡿᚤ㔞ඖ⣲ࡢศᕸ࡜ᣲື㸪㸷㸬㕥ᮌ⨾ဏ㸪ᮏከ↷ᖾ㸹ఀໃ‴୪ࡧ࡟኱㜰‴ᾏᗏ

➨ 44 ᅇ࢔࢖ࢯࢺ࣮ࣉ࣭ᨺᑕ⥺◊✲Ⓨ⾲఍せ᪨㞟㸪ሁ✚≀࡟࠾ࡅࡿᚤ㔞ඖ⣲ࡢᣲື࡜ሁ✚⎔ቃ㸪2006

p.98㸪2007ᖺᗘ᪥ᮏᆅ⌫໬Ꮫ఍➨ 53 ᅇᖺ఍ㅮ₇せ᪨㞟㸪㸵㸬Ọ⏣ᐶ㸪ᮏከ↷ᖾ㸹⍞ᾉᒙ⩌࡟࠾ࡅࡿᆅ⌫໬Ꮫⓗ⎔ቃࡢኚ໬࡟క࠺ᚤ㔞ඖ⣲ࡢศᕸ࡜ᣲື㸪2007

p.111㸪2006

3-11

ᖺ ᗘ᪥ᮏᆅ⌫໬Ꮫ఍➨ 54 ᅇᖺ఍ㅮ₇せ᪨㞟㸪
p.181㸪2007- 362 -

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JAEA-Review 2013-039

3-12㺀ள㖄Ḟஈ≧ែ࡟࠾ࡅࡿ⫢⣽⬊࠾ࡼࡧ⮅⣽⬊୰ࡢྍ⁐ᛶࢱࣥࣃࢡ㉁ࡢᵓ㐀ኚ໬㺁Effects of Zn deficiency on metalloproteins in hepatic and pancreatic cells▮ỌㄔேࠊⳢ἟ⱥኵࠊ㔝ཱྀᇶᏊࠊୖᓥ῟ឿࠊᕝᓥ⨾ᬛᏊࠊᮧᯇ ⯟ࠊᒣ㔝 ႐ࠊᕝཱྀ๛ᗈࠊἙᮧ ᪸ࠊୗᒣᘯ㧗ࠊᒣᮏ ╩㟼ᒸ኱Ꮫ⌮Ꮫ㒊
Makoto YANAGA, Hideo SUGANUMA, Motoko NOGUCHI, Junji KAMISHIMA,
Michiko KAWASHIMA, Wataru MURAMATSU, Yoshi YAMANO,
Takehiro KAWAGUCHI, Akira KAWAMURA, Hirotaka SHIMOYAMA, Osamu YAMAMOTO
Faculty of Science, Shizuoka University㸦㸯㸧 ࡣࡌࡵ࡟
ᡃࠎࡢయࡣࠊ୺࡜ࡋ࡚ࠊⅣ⣲ࡸ㓟⣲ࠊỈ⣲࡞࡝ࠊ᭷ᶵ≀ࢆᵓᡂࡍࡿඖ⣲࡟ࡼࡾᵓᡂࡉࢀ࡚࠸ࡿࠋࡲࡓࠊ
⏕࿨άື࡟ࡣࠊሷศࠊࡍ࡞ࢃࡕࢼࢺ࣒ࣜ࢘ࡸ࢝ࣜ࢘
࣒ࠊሷ⣲࡞࡝ࡢ㟁ゎ㉁ࡶᚲせ࡜ࡉࢀࠊࡉࡽ࡟ࠊ❅⣲ࡸ࢖࢜࢘ࠊࣜࣥ࡞࡝ࡣࠊࢱࣥࣃࢡ㉁ࡸ᰾㓟ࡢᵓᡂᡂศ࡜࡞ࡗ࡚࠸ࡿࠋᡃࠎࡢయ࡟ࡣࠊࡇࢀࡽࡢඖ⣲ࡢ௚ࠊࡑࡢ㔞ࡣᚤ㔞࡛ࡣ࠶ࡿࡀࠊᚲ㡲ᛶࡢ㧗࠸ඖ⣲ࡀከᩘྵࡲࢀ࡚࠸ࡿࠋࡑࡢ୰࡛ࡶள㖄ࡣࠊᏑᅾ㔞ࡣ㕲࡟ḟ࠸࡛㸰␒┠࡛࠶ࡿࡀࠊࡑࡢᶵ⬟ࡢከᵝᛶ࠿ࡽࠊࡶࡗ
࡜ࡶᚲ㡲ᛶࡢ㧗࠸⏕యᚤ㔞ඖ⣲࡛࠶ࡿ࡜ゝ࠼ࡼ࠺ࠋࡇࡢள㖄ࡀḞஈࡍࡿ࡜࿡ぬ࣭Ⴅぬ㞀ᐖࠊᛶ⭢ᶵ⬟పୗࠊ⓶⭵㞀ᐖࠊච␿ᶵ⬟పୗࠊᡂ㛗㞀ᐖ࡞࡝ࡢ⑕
≧ࡀ⌧ࢀࡿࡇ࡜ࡀ࠶ࡿࠋள㖄Ḟஈࡢཎᅉࡢ୍ࡘ࡜ࡋ
࡚㣗㣵୰ࡢள㖄୙㊊ࡀ࠶ࡆࡽࢀࡿࡀࠊᡃࠎࡣࠊࡇࡢ
㣗㣵୰ࡢள㖄୙㊊࡟క࠺ள㖄Ḟஈࢆᑐ㇟࡜ࡋࠊள㖄Ḟஈࡀ㔠ᒓ⤖ྜࢱࣥࣃࢡ㉁ࠊ≉࡟ࠊள㖄⤖ྜࢱࣥࣃ
ࢡ㉁ࢆ௓ࡋ࡚௚ࡢඖ⣲ࡢᣲື࡟୚࠼ࡿᙳ㡪࡟ࡘ࠸᳨࡚ウࡋ࡚ࡁ࡚࠸ࡿࠋࡇࢀࡲ࡛ࠊள㖄Ḟஈ㣵࠾ࡼࡧᑐ↷㣵࡛㣫⫱ࡋࡓ࣐࢘ࢫࡢྛ⮚ჾ࠾ࡼࡧ⤌⧊࡟ࡘ࠸࡚ࠊ
ᶵჾ୰ᛶᏊᨺᑕ໬ศᯒἲ࡟ࡼࡾ✀ࠎࡢᚤ㔞ඖ⣲ࡢᐃ㔞ࢆ⾜࠸ࠊẚ㍑᳨ウࡋ࡚ࡁࡓࠋࡑࡢ⤖ᯝࠊእほୖ࠾ࡼࡧ⤌⧊Ꮫⓗほᐹ࡟࠾࠸࡚ࡶள㖄Ḟஈ࡟ࡼࡿᙳ㡪ࡀㄆࡵࡽࢀ࡞࠸ሙྜ࡟࠾࠸࡚ࠊள㖄⃰ᗘ࡟㛵ࡋ࡚ࡣࠊள㖄Ḟஈ⩌ࡢ㦵ࡸ⮅⮚࡛ࡣ᭷ព࡟పୗࡋ࡚࠸ࡓࡀࠊ
ࡑࡢ௚ࡢ⮚ჾ࡛ࡣ㢧ⴭ࡞⃰ᗘపୗࡣㄆࡵࡽࢀ࡞࠿ࡗ
ࡓࠋࡲࡓࠊࢥࣂࣝࢺ⃰ᗘ࡟㛵ࡋ࡚ࡣࠊள㖄Ḟஈ࣐࢘ࢫࡢ඲࡚ࡢ⮚ჾ࣭⤌⧊࡛ቑຍࡋ࡚࠸ࡓࠋ
ࡇࢀࡽࡇ࡜ࡣࠊ㢧ⴭ࡞ள㖄Ḟஈ⑕≧ࡀㄆࡵࡽࢀࡿ
௨๓ࡢள㖄⤖ྜࢱࣥࣃࢡ㉁࡞࡝ࡢ⏕యෆ㔠ᒓ⤖ྜ≀㉁ࡢኚ໬ࢆ♧ࡋ࡚࠸ࡿࡶࡢ࡜⪃࠼ࡽࢀࡿࠋࡑࡇ࡛ࠊ
ᮏ◊✲࡛ࡣࠊள㖄Ḟஈ⑕≧ࡀ⌧ࢀࡿ௨๓࡟ኚ໬ࡍࡿ

⏕య≀㉁ࠊ≉࡟㔠ᒓ⤖ྜࢱࣥࣃࢡ㉁ࡀ⣽⬊ෆࡢ࡝ࡢ㒊ศ࡟࠶ࡿ࠿ࢆ᳨⣴ࡍࡿࡓࡵ࡟ࠊ⫢⣽⬊࠾ࡼࡧ⮅⣽⬊࡟ࡘ࠸࡚㐲ᚰศ㞳ἲ࡟ࡼࡿ⣽⬊ศ⏬ࢆ⾜࠸ࠊྛ⏬
ศ࡟ࡘ࠸࡚ࠊᶵჾ୰ᛶᏊᨺᑕ໬ศᯒࢆ⾜࠺ࡇ࡜࡜ࡋ
ࡓࠋ㸦㸰㸧ᐇ㦂
㸰㸫㸯 ౪ヨື≀࠾ࡼࡧ⣽⬊ศ⏬㸶㐌㱋ࡢ㹇㹁㹐⣔࢜ࢫ࣐࢘ࢫࢆࠊள㖄Ḟஈ⩌࡜ᑐ↷⩌ࡢ㸰⩌࡟ศࡅࠊள㖄Ḟஈ⩌࡟ࡣள㖄Ḟஈ㣵࠾ࡼࡧ㉸⣧Ỉࢆࠊࡲࡓࠊᑐ↷⩌࡟ࡣᑐ↷㣵 ள㖄Ḟஈ㣵࡟ሷᇶᛶⅣ㓟ள㖄ࢆῧຍࡋࡓ㣫ᩱ ࠾ࡼࡧ㉸⣧Ỉࢆ୚࠼࡚㣫⫱ࡋࡓࠋ࡞࠾ࠊྛ㣫ᩱࡣࠊ ᰴ ᪥ᮏࢡࣞ࢔࡟
ㄪ〇ࢆ౫㢗ࡋࡓࡶࡢࢆ౑⏝ࡋࡓࠋྛࠎࡢ࣐࢘ࢫ࡟ࡘ
࠸࡚ࠊ㸯㐌㛫ࡢ㣫⫱ࡢᚋࠊ࢚࣮ࢸࣝ㯞㓉ୗ࡟࠾࠸࡚ࠊ
⮚ჾࡢ᦬ฟࢆ⾜ࡗࡓࠋ᦬ฟࡋࡓ⫢⮚ࡸ⮅⮚ࢆ
HEPES ⦆⾪ᾮ୰࡟࡚࣍ࣔࢪࢼ࢖ࢬࡋࠊࡑࡢᚋࠊ㸳ᅇࡢ㐲ᚰ᧯స 50×g 7 ศࠊ1,000×g 10 ศࠊ
9,000×g 10
ศࠊ30,000×g 30 ศࠊ105,000×g 65 ศ ࡟ࡼࡾ㠀◚ቯ⣽⬊ࠊ᰾⏬ศࠊ࣑ࢺࢥࣥࢻࣜ࢔⏬ศࠊࣜࢯࢯ࣮࣒
⏬ศࠊ࣑ࢡࣟࢯ࣮࣒⏬ศ࠾ࡼࡧࢧ࢖ࢺࢰࣝ⏬ศࡢ㸴ࡘࡢ⏬ศ࡟ศ㞳ࡋࡓࠋศ㞳ࡋࡓྛ⏬ศࡣࠊ⛗㔞ࡋࡓᚋ࡟෾⤖஝⇱ࡋࠊศᯒヨᩱ࡜ࡋࡓࠋ࡞࠾ࠊ⮅⮚࡟ࡘ࠸࡚ࡣࠊࡑࡢ኱ࡁࡉࡀᑠࡉ࠸ࡓࡵࠊ㸶ಶయศࢆྜࢃ
ࡏ࡚࣍ࣔࢪࢼ࢖ࢬ࠾ࡼࡧ㐲ᚰ᧯సࢆ⾜ࡗ࡚ࠊศᯒヨᩱ࡜ࡋࡓࠋ㸰㸫㸰 ↷ᑕ࠾ࡼࡧ ᐃ ෾⤖஝⇱ࡋࡓྛ⏬ศࢆ࣏࢚ࣜࢳࣞࣥ⿄࡛஧㔜ᑒධࡲࡓࡣ୕㔜ᑒධࡋࠊ↷ᑕヨᩱ࡜ࡋࡓࠋᶆ‽ヨᩱ࡟ࡣࠊ
NIST SRM 1577b Bovine Liver ࠾ࡼࡧཎᏊ྾ගศ
ᯒ⏝ Mg ᶆ‽⁐ᾮࡢ୍ᐃ㔞ࢆࢁ⣬ୖ࡟⁲ୗࡋ஝⇱ࡉ◊✲᪋タ࣭⿦⨨                ◊✲ศ㔝
JRR-3 Ẽ㏦↷ᑕタഛ(PN-1, PN-3)       ⏕యヨᩱࡢᨺᑕ໬ศᯒ
JRR-4 Ẽ㏦⟶࠾ࡼࡧ T ࣃ࢖ࣉ- 363 -

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JAEA-Review 2013-039

ࡏࡓࡶࡢࡢࡑࢀࡒࢀࢆࠊ࣏࢚ࣜࢳ࡛ࣞࣥ஧㔜ᑒධࡲࡓࡣ୕㔜ᑒධࡋࡓࡶࡢࢆ⏝࠸ࡓࠋ ⇕୰ᛶᏊ↷ᑕࡣࠊJRR-3M ࡲࡓࡣ JRR-4 ࡟࠾࠸࡚ࠊ┠ⓗඖ⣲࡟ᛂࡌ࡚㸰✀㢮ࡢ↷ᑕࢆ⾜ࡗࡓࠋࡍ࡞
ࢃࡕࠊ▷ᑑ࿨᰾✀࡟ࡼࡾᐃ㔞ࡍࡿඖ⣲࡟ࡘ࠸࡚ࡣࠊ
JRR-3M ᨺ ᑕ ໬ ศ ᯒ ⏝ ↷ ᑕ タ ഛ PN-3 ࡲ ࡓ ࡣ
JRR-4 Ẽ㏦⟶࡟࡚㸯ศ㛫ࡢ↷ᑕࢆ⾜ࡗࡓࠋࡲࡎࠊ
MgࠊCl ࠾ࡼࡧ Cu ࡢᐃ㔞ࢆ┠ⓗ࡜ࡋ࡚ࠊ↷ᑕ㸰㹼
10 ศᚋ࡟㧗⣧ᗘ Ge ༙ᑟయ᳨ฟჾ࡟࡚ 120㹼300 ⛊㛫ࡢȚ⥺ࢫ࣌ࢡࢺ࣓ࣟࢺ࣮ࣜࢆ⾜࠸ࠊḟ࡟ࠊNa ࠾
ࡼࡧ Mn ࡢᐃ㔞ࡢࡓࡵࠊ㸯ᅇ┠ࡢ ᐃ࠿ࡽ 60㹼150ศᚋ࡟ࠊ෌ᗘࠊ250㹼600 ⛊㛫ࡢ ᐃࢆ⾜ࡗࡓࠋ ࡲࡓࠊ㛗ᑑ࿨᰾✀࡟ࡼࡾᐃ㔞ࡍࡿඖ⣲ FeࠊCoࠊ
ZnࠊSe ࠾ࡼࡧ Rb ࡢᨺᑕ໬ࡢࡓࡵ࡟ࠊJRR-3M Ẽ㏦↷ᑕタഛ PN-1 ࡟࡚ 20 ศ㛫ࡢ↷ᑕࡲࡓࡣ JRR-4
T-ࣃ࢖ࣉ࡟࡚ 30㹼40 ศ㛫ࡢ↷ᑕࢆ⾜࠸ࠊ10㹼60 ᪥
ᚋ࡟ 3㹼48 ᫬㛫ࡢȚ⥺ ᐃࢆ⾜ࡗࡓࠋ ࡲࡓࠊࡑࡢ௚ࡢ⣽⬊ᡂศ࡟࠾࠸࡚ࡶள㖄Ḟஈ⩌࡜ᑐ↷⩌ࡢ㛫࡛ள㖄⃰ᗘ࡟᭷ព࡞ᕪࢆㄆࡵࡿࡇ࡜ࡣ࡛
ࡁ࡞࠿ࡗࡓࠋ୍᪉ࠊ㐣ཤ࡟⾜ࡗࡓᐇ㦂⤖ᯝࡼࡾࠊ㸶㐌㱋࠿ࡽ㸱㐌㛫㣫⫱ࡋࡓ࣐࢘ࢫࡢ⫢⮚࡟ࡘ࠸࡚ࠊᮏ
◊✲࡜ྠᵝࡢᐇ㦂ࢆ⾜ࡗࡓ࡜ࡁࠊள㖄Ḟஈ⩌࡛ࡣᑐ↷⩌࡜ẚ࡭࡚ࠊ࣑ࢺࢥࣥࢻࣜ࢔ࠊ࣑ࢡࣟࢯ࣮࣒ࠊࢧ
࢖ࢺࢰࣝࡢ㸱ࡘࡢ⏬ศ࡛ள㖄⃰ᗘࡢῶᑡࡀぢࡽࢀࡿࡇ࡜ࡀࢃ࠿ࡗ࡚࠸ࡿࠋࡇࡢࡇ࡜࠿ࡽࠊ㣫⫱㸯㐌㛫ࡢ
᫬Ⅼ࡛ࡣ⫢⮚ࡢྛ⣽⬊ᡂศ୰࡛ࡣࠊள㖄⃰ᗘࡢኚ໬ࡣ㉳ࡇࡗ࡚࠸࡞࠸࠿ࠊࡲࡓࡣ㠀ᖖ࡟ࢃࡎ࠿࡞ࡶࡢ࡛
࠶ࡿࡀࠊள㖄Ḟஈ≧ែࡢᮇ㛫ࡀ㛗ࡃ⥆ࡃ࡟ࡘࢀࠊࢧ
࢖ࢺࢰࣝ⏬ศ࡞࡝࡛ள㖄⃰ᗘࡀῶᑡࡋ࡚࠸ࡃ࡜⪃࠼ࡽࢀࡿࠋ ḟ࡟ࠊ⫢⣽⬊ࡢྛ⣽⬊ᡂศ୰ࡢࢥࣂࣝࢺ⃰ᗘࡢศᯒ⤖ᯝࢆᅗ㸰࡟♧ࡍࠋ㸦㸱㸧⤖ᯝ࠾ࡼࡧ⪃ᐹ㸱㸫㸯 ⫢⮚⫢⣽⬊ࡢྛ⣽⬊ᡂศ୰ࡢள㖄⃰ᗘࡢศᯒ⤖ᯝࢆᅗ
1 ࡟♧ࡍࠋ

ᅗ㸰 㸶㐌㱋࠿ࡽ㸯㐌㛫㣫⫱ࡋࡓ࣐࢘ࢫ⫢⮚ࡢྛ⣽⬊ᡂศ୰࡟࠾ࡅࡿࢥࣂࣝࢺ⃰ᗘ㸹)㠀◚ቯ⣽⬊ࠊ)᰾⏬ศࠊ)࣑ࢺࢥࣥࢻࣜ࢔⏬ศࠊ)ࣜࢯࢯ࣮࣒⏬ศࠊ)࣑ࢡ
ࣟࢯ࣮࣒⏬ศࠊ)ࢧ࢖ࢺࢰࣝ⏬ศᅗ㸯 㸶㐌㱋࠿ࡽ㸯㐌㛫㣫⫱ࡋࡓ࣐࢘ࢫ⫢⮚ࡢྛ⣽⬊ᡂศ୰࡟࠾ࡅࡿள㖄⃰ᗘ㸹)㠀◚ቯ⣽⬊ࠊ)᰾⏬ศࠊ)࣑
ࢺࢥࣥࢻࣜ࢔⏬ศࠊ)ࣜࢯࢯ࣮࣒⏬ศࠊ)࣑ࢡࣟࢯ࣮࣒⏬ศࠊ)ࢧ࢖ࢺࢰࣝ⏬ศ௨๓࡟⾜ࡗࡓࠊᮏ◊✲࡜ྠ᮲௳࡛㣫⫱ࡋࡓ࣐࢘ࢫ⫢⮚୰ள㖄⃰ᗘࡢศᯒ⤖ᯝ࡛ࡣࠊ㸶㐌㱋࠿ࡽ㸯㐌㛫㣫⫱ࡋࡓሙྜ࡟࠾࠸࡚ࠊள㖄Ḟஈ⩌ࡢள㖄⃰ᗘࡀࢃࡎ࠿࡟పୗࡋ࡚࠸ࡓࠋࡋ࠿ࡋࠊ௒ᅇࠊศ⏬ࡋ࡚࠸࡞࠸
⫢⮚࡜ྠᵝ࡟⪃࠼ࡿࡇ࡜ࡀ࡛ࡁࡿ㠀◚ቯ⣽⬊ࡢᐃ㔞್࡟ࡘ࠸࡚ぢࡿ࡜ࠊ୧⩌㛫࡟᭷ព࡞ᕪࢆㄆࡵࡿࡇ࡜
ࡣ࡛ࡁ࡞࠿ࡗࡓࠋࡇࢀࡣࠊ」ᩘࡢ⫢⮚࡟ࡘ࠸࡚ࡢศ
⏬᧯సࢆ᏶඲࡟ྠࡌࡼ࠺࡟⾜࠺ࡇ࡜ࡣᅔ㞴࡛࠶ࡿࡓࡵࠊࡶ࡜ࡶ࡜ࢃࡎ࠿࡛࠶ࡗࡓᕪࢆ࡜ࡽ࠼ࡿࡇ࡜ࡀ࡛
ࡁ࡞࠿ࡗࡓࡓࡵ࡜⪃࠼࡚࠸ࡿࠋ

ࢥࣂࣝࢺ⃰ᗘࡣࠊள㖄Ḟஈ⩌ࡢ㠀◚ቯ⣽⬊ࠊࣜࢯࢯ࣮࣒⏬ศࠊࢧ࢖ࢺࢰࣝ⏬ศ࡟࠾࠸࡚᭷ព࡞⃰ᗘቑຍࡀぢࡽࢀࡓࠋࡲࡓࠊࡑࡢ௚ࡢ⏬ศ࡟ࡘ࠸࡚ࡶ᭷ពỈ‽࡟ࡣ㐩ࡋ࡞࠿ࡗࡓࡀࠊ࡝ࡢ⏬ศ࡟࠾࠸࡚ࡶள㖄Ḟஈ⩌࡛⃰ᗘࡢቑຍഴྥࡀぢࡽࢀࡓࠋ௨๓࡟⾜ࡗࡓ㸶㐌㱋࠿ࡽ㸱㐌㛫㣫⫱ࡋࡓ࣐࢘ࢫࡢ⫢⮚ࡢศᯒ࡟࠾࠸
࡚ࡣࠊ඲࡚ࡢ⏬ศ࡛ள㖄Ḟஈ⩌࡛ࡢࢥࣂࣝࢺ⃰ᗘࡢ᭷ព࡞ቑຍࡀぢࡽࢀࡓࠋள㖄Ḟஈ⩌㛫࠾ࡼࡧᑐ↷⩌㛫࡛ࠊ㸯㐌㣫⫱᫬ࡢᐃ㔞್࡜㸱㐌㣫⫱᫬ࡢᐃ㔞್࡜ࢆẚ㍑ࡋࡓ࡜ࡇࢁࠊ㣫⫱㐌࡟ࡼࡿࢥࣂࣝࢺ⃰ᗘࡢኚ໬ࡣ୧⩌࡜ࡶ࡯࡜ࢇ࡝ぢࡽࢀ࡞࠿ࡗࡓࠋࡇࡢࡇ࡜࠿
ࡽࠊ㐌㣫⫱᫬࡟ࡶ඲࡚ࡢ⏬ศ࡟࠾࠸࡚ள㖄Ḟஈ⩌࡛ࢥࣂࣝࢺ⃰ᗘࡢቑຍࡀ㉳ࡁ࡚࠸ࡿ࡜⪃࠼ࡽࢀࡿࠋ
ᮏᐇ㦂࡟࠾࠸࡚᭷ពᕪࡢぢࡽࢀ࡞࠿ࡗࡓ᰾⏬ศ࡞࡝࡟ࡘ࠸࡚ࡶࠊศᯒヨᩱᩘࢆࡉࡽ࡟ቑࡸࡍࡇ࡜࡟ࡼࡾࠊ
᭷ពᕪࡀ☜ㄆ࡛ࡁࡿ࡜⪃࠼ࡽࢀࡿࠋࡲࡓࠊ⫢⮚ࡢ඲ศᯒ࡟࠾࠸࡚ࡣࠊ㸱㐌㣫⫱ࡋࡓள㖄Ḟஈ⩌࡛ࡣ㸯㐌㣫⫱ࡢࡶࡢࡼࡾࡶࢃࡎ࠿࡟ࢥࣂࣝࢺ⃰ᗘࡢቑຍࡀぢ

3-12- 364 -

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JAEA-Review 2013-039

ࡽࢀ࡚࠸ࡓࠋࡋ࠿ࡋࠊ௒ᅇ⾜ࡗࡓᐇ㦂࡟࠾࠸࡚ࡣࠊ
࡝ࡢ⏬ศ࡟࠾࠸࡚ࡶ㸯㐌㣫⫱࡜㸱㐌㣫⫱ࡢ㛫࡛⃰ᗘᕪࢆぢฟࡍࡇ࡜ࡣ࡛ࡁ࡞࠿ࡗࡓࠋࡇࢀࡣࠊศ⏬᧯సࢆ⾜ࡗࡓࡇ࡜࡟ࡼࡾࠊศᯒヨᩱ࡜ࡋ࡚౪ࡍࡿࡇ࡜ࡀ
࡛ࡁࡿヨᩱࡀᑡ࡞ࡃ࡞ࡗࡓࡇ࡜ࡸࠊヨᩱ㛫ࡢࡤࡽࡘࡁࡀ኱ࡁࡃ࡞ࡗࡓࡓࡵࡔ࡜⪃࠼ࡽࢀࡿࠋ
⏕యෆ࡟Ꮡᅾࡍࡿࢥࣂࣝࢺࡢ໬Ꮫᙧ࡜ࡋ࡚ࡣࠊࢥ
ࣂ࣑ࣛࣥ➼ࡢࣅࢱ࣑ࣥ %⩌ࡢᙧ࡛Ꮡᅾࡍࡿ࠿ࠊ࠶ࡿ
࠸ࡣ↓ᶵ࢖࢜ࣥ࡜ࡋ࡚ࢱࣥࣃࢡ㉁࡜⤖ྜࡋ࡚Ꮡᅾࡋ
࡚࠸ࡿࡇ࡜ࡀ⪃࠼ࡽࢀࡿࠋࢥࣂࣝࢺࢆྵࡴ㓝⣲࡜ࡋ࡚ࡣࢺࣛࣥࢫ࢝ࣝ࣎࢟ࢩ࣮ࣛࢮࡸ࢔࣑ࣀ࣌ࣉࢳࢲ࣮
ࢮ࡞࡝ࡀ࠶ࡿࡀࠊ㓝⣲άᛶ࡟ᚲせ࡞ࡢࡣ௚ࡢ㔠ᒓ࡛࠶ࡿࡇ࡜࠿ࡽࠊ௒ᅇࡢᐇ㦂⤖ᯝ࡜ࡇࢀࡽ㓝⣲࡜ࡢ㛫ࡢ㛵ಀࢆ㆟ㄽࡍࡿࡇ࡜ࡣ㞴ࡋ࠸࡛࠶ࢁ࠺ࠋࡲࡓࠊ=Q
ࢆ &R࡟⨨᥮ࡋࡓሙྜ࡟ࠊάᛶࢆಖࡘ࠶ࡿ࠸ࡣάᛶ
ࢆቑ኱ࡉࡏࡿள㖄㓝⣲ࡀᩘከࡃሗ࿌ࡉࢀ࡚࠸ࡿࠋࡉ
ࡽ࡟ࠊᚤ⏕≀㉳※ࡢள㖄㓝⣲ࡢ୰࡟ࡣࠊῧຍࡋࡓ &Rࡀ㓝⣲୰ࡢ =Q࡜⨨᥮ࡍࡿࡇ࡜࡞ࡃྲྀࡾ㎸ࡲࢀ࡚ࠊ㓝⣲ࢆάᛶ໬ࡉࡏࡿࡶࡢࡶ▱ࡽࢀ࡚࠸ࡿࠋࡇࡢࡇ࡜
࠿ࡽࠊ㣗㣵୰ࡢள㖄ࡀḞஈࡋࡓሙྜ࡟ࡣࠊࢥࣂ࣑ࣛ
ࣥࡀ㣗㣵࠿ࡽ✚ᴟⓗ࡟ྲྀࡾ㎸ࡲࢀࡓࡾࠊయእ࡬ࡢ᤼
ฟࡀᢚไࡉࢀࡓࡾࡍࡿ࡜࠸࠺ࡼࡾࡣࠊள㖄⤖ྜࢱࣥ
ࣃࢡ㉁୰ࡢள㖄࡜ࢥࣂࣝࢺࡀ⨨᥮ࡍࡿࠊ࠶ࡿ࠸ࡣࢥ
ࣂࣝࢺࡀ௜ຍࡍࡿࡇ࡜࡟ࡼࡾࠊࡑࡢ㓝⣲άᛶࢆ⥔ᣢࡲࡓࡣୖ᪼ࡉࡏࡿ࡞࡝ࡢാࡁࢆࡋ࡚࠸ࡿྍ⬟ᛶࡀ⪃࠼ࡽࢀࡿࠋள㖄㓝⣲୰ࡢள㖄࡜⨨᥮ࡀ㉳ࡁࡓሙྜ࡟
ࡣள㖄⃰ᗘࡀῶᑡࡍࡿࡇ࡜ࡀ⪃࠼ࡽࢀࡿࡀࠊ⫢⮚୰ࡢࢥࣂࣝࢺ⃰ᗘࡣள㖄⃰ᗘࡢ ศࡢ ௨ୗ࡛࠶
ࡿࡓࡵࠊ௬࡟ቑຍࡋࡓࢥࣂࣝࢺࡢ඲࡚ࡀள㖄࡜⨨᥮ࡋࡓሙྜ࡟࠾࠸࡚ࡶࠊள㖄⃰ᗘࡢῶᑡࢆ᳨ฟࡍࡿࡇ
࡜ࡣ㞴ࡋ࠸࡜⪃࠼ࡽࢀࡿࠋࡲࡓࠊள㖄⃰ᗘࡀῶᑡࡋ
࡚࠸࡞࠸ẁ㝵࡟࠾࠸࡚ࡶࢥࣂࣝࢺ⃰ᗘࡀቑຍࡋ࡚࠸
ࡿࡇ࡜࠿ࡽࠊ⣽⬊ෆࡢள㖄⃰ᗘࢆಖࡘࡓࡵࡢㄪ⠇ᶵ⬟࡟ࢥࣂࣝࢺࡀ㛵୚ࡋ࡚࠸ࡿྍ⬟ᛶࡶ⪃࠼ࡽࢀࡿࠋ
㸱㸫㸰 ⮅⮚⮅⣽⬊ࡢศᯒࡣࠊᐇ㦂ࡢ❶࡛グࡋࡓࡼ࠺࡟ࠊࡑࡢ
⮚ჾࡢᑠࡉࡉࡢࡓࡵࠊ㸶ಶయศࢆ㸯ヨᩱ࡜ࡋ࡚ศᯒ
ࢆ⾜ࡗࡓࠋ෌⌧ᛶࡀᚓࡽࢀࡓ⤖ᯝ࡜ࡋ࡚ࠊྍ⁐ᛶࢱ
ࣥࣃࢡ㉁ࡀᏑᅾࡍࡿࢧ࢖ࢺࢰࣝ⏬ศ࡛ࡣࠊள㖄Ḟஈ⩌ࡢள㖄⃰ᗘࡀపୗࡋࠊࢥࣂࣝࢺࡢ⃰ᗘࡀቑຍࡋ࡚
࠸ࡓࠋྍ⁐ᛶ⏬ศ௨እࡢ⏬ศ࡟ࡘ࠸࡚ࡣࠊள㖄⃰ᗘࡣ࣑ࢡࣟࢯ࣮࣒⏬ศࢆ㝖ࡃ5⏬ศ࡟࠾࠸࡚ࠊள㖄Ḟஈ⩌࡛ᑐ↷⩌ࡢࡑࢀࡼࡾࡶῶᑡࡋ࡚࠸ࡓࠋࡑࡢ࡯࠿
ࡢඖ⣲࡟ࡘ࠸࡚ࡣࠊ᭷ព࡞ᕪࢆぢࡿࡇ࡜ࡀ࡛ࡁ࡞࠿
ࡗࡓࠋࢧ࢖ࢺࢰࣝ⏬ศ࡟ࡣከࡃࡢࢱࣥࣃࢡ㉁ࡀᏑᅾ
ࡍࡿࡇ࡜࠿ࡽࠊࢧ࢖ࢺࢰࣝ⏬ศ୰ࡢࢱࣥࣃࢡ㉁ᵓ㐀࡟ఱࡽ࠿ࡢᵓ㐀ኚ໬ࡀ㉳ࡇࡿྍ⬟ᛶࡀ♧၀ࡉࢀࡓࠋ

ࡑࡢ⪃࠼ࡽࢀࡿྍ⬟ᛶ࡜ࡋ࡚ࡣࠊள㖄⤖ྜࢱࣥࣃࢡ㉁ࡢᾘኻࠊள㖄ࡀ㐟㞳ࡋࡓ࢔࣏ࢱࣥࣃࢡ㉁࡜ࡋ࡚Ꮡ
ᅾࠊள㖄࡜௚ࡢ㔠ᒓ࡜ࡢ⨨᥮ࡀ࠶ࡿࠋ ࡑࡇ࡛ࠊࢧ࢖ࢺࢰࣝ⏬ศ୰ࡢࢱࣥࣃࢡ㉁࡟ࡘ࠸࡚ࠊ
SDS-PAGE ࡸ㸰ḟඖ㟁ẼὋືࡢ௚ࠊࢤࣝࢡ࣐ࣟࢺࢢ
ࣛࣇ࢕࣮࡟ࡼࡿศᏊࢧ࢖ࢬูࡢศ㞳࡜ศ㞳ࡋࡓྛࣇࣛࢡࢩࣙࣥࡢศᯒ➼࡟╔ᡭࡋࡓࠋ௒ᚋࡣࠊࡇࢀࡽࡢ
⤖ᯝࢆ㋃ࡲ࠼࡚ࠊ㣗㣵୰ࡢள㖄୙㊊࡜⮅⮚୰ࡢ㔠ᒓࢱࣥࣃࢡ㉁ࡢኚ໬࡜ࡢ㛵ಀࢆ᳨ウࡋ࡚࠸ࡃணᐃ࡛࠶
ࡿࠋ㸦㸲㸧◊✲ᡂᯝ Ꮫ఍Ⓨ⾲
1 ᕝᓥ⨾ᬛᏊࠊୖᓥ῟ឿࠊᯇୗ࿴㤿ࠊⓙྜྷ㱟஧ࠊ㔝ཱྀᇶᏊࠊⳢ἟ⱥኵࠊ▮Ọㄔேࠊࠕள㖄Ḟஈ࣐࢘ࢫࡍ࠸⮚⣽⬊୰ࡢᚤ㔞ඖ⣲⃰ᗘࡢᐃ㔞㺁ࠊ2006 ᪥ᮏ ᨺ ᑕ ໬ Ꮫ ఍ ᖺ ఍ ࣭ ➨ 50 ᅇ ᨺ ᑕ ໬ Ꮫ ウ ㄽ ఍2006 ᖺ 10 ᭶ Ỉᡞࠊᮾᾏ . 
2 ୖᓥ῟ឿࠊᑠᮌ㈗᠇ࠊⓙྜྷ㱟஧ࠊᕝᓥ⨾ᬛᏊࠊ⾰ᕝಙஅࠊⳢ἟ⱥኵࠊ㔝ཱྀᇶᏊࠊ▼ᕝ຾฼ࠊୡⰋ
⪔୍㑻ࠊ▮Ọㄔேࠊࠕள㖄Ḟஈ࣐࢘ࢫ⫢⣽⬊ᡂศ୰࡟࠾ࡅࡿᚤ㔞ඖ⣲⃰ᗘ࠾ࡼࡧ㔠ᒓࢱࣥࣃࢡ㉁ࡢ
ኚ໬㺁ࠊ2006 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍࣭➨ 50 ᅇᨺᑕ໬Ꮫウㄽ఍ 2006 ᖺ 10 ᭶ Ỉᡞࠊᮾᾏ . 㸱 ᮧᯇ ⯟ࠊୖᓥ῟ឿࠊᕝᓥ⨾ᬛᏊࠊᒣ㔝 ႐ࠊⳢ἟ⱥኵࠊ㔝ཱྀᇶᏊࠊ▮Ọㄔேࠊࠕள㖄Ḟஈึᮇ࡟࠾ࡅࡿ࣐࢘ࢫ⫢⮚୰ࡢᚤ㔞ඖ⣲⃰ᗘࡢኚ໬㺁ࠊ
2007 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍࣭➨ 51 ᅇᨺᑕ໬Ꮫウㄽ
఍ 2007 ᖺ 9 ᭶ 㟼ᒸ . 㸲 ᮧᯇ ⯟ࠊୖᓥ῟ឿࠊᕝᓥ⨾ᬛᏊࠊᒣ㔝 ႐ࠊⳢ἟ⱥኵࠊ㔝ཱྀᇶᏊࠊ▮Ọㄔேࠊࠕள㖄Ḟஈึᮇ࡟࠾ࡅࡿ࣐࢘ࢫ⫢⮚୰ࡢᚤ㔞ඖ⣲⃰ᗘ࠾ࡼࡧࢱࣥ
ࣃࢡ㉁ࡢኚ໬㺁ࠊ2008 ᪥ᮏᨺᑕ໬Ꮫ఍ᖺ఍࣭➨ 52ᅇᨺᑕ໬Ꮫウㄽ఍ 2008 ᖺ 9 ᭶ ᗈᓥ . 
Publications1 J. Kamishima, T. Ogi, R. Minayoshi, N. Kinugawa,H. Suganuma, M. Noguchi, K. Ishikawa, M. Yanaga,“Determination of trace elements in hepatocyte of zinc
deficient mice by means of INAA”, J. Radioanal. Nucl.
Chem. , 272, 419-422(2007).

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JAEA-Review 2013-039

3-13ᨺᑕ໬ศᯒἲࢆ⏝࠸ࡓᶞᮌᖺ㍯ゎᯒ࡟ࡼࡿ㔠ᒓඖ⣲ࡢ⎔ቃືែே㛫⎔ቃ኱Ꮫ

∦ᒣᖾኈ ࠊ㛗஭ṇ༤ࠊ㟷ᮌ 㐩ி㒔኱Ꮫ ኱Ꮫ㝔㎰Ꮫ◊✲⛉ᒸ⏣┤⣖ᮾி㎰ᕤ኱Ꮫ ␃Ꮫ⏕ࢭࣥࢱ࣮ᕝ➃ⰋᏊ

Environmental Investigation of Metallic Elements by Dendrochronology with Activation Analysis
Yukio Katayama1, Masahiro Nagai1, Toru Aoki1, Naoki Okada2, Yoshiko Kawabata3
The Division of Human Environment, University of Human Environments, 2Graduate School of Agriculture, Kyoto

1

University,

3

International Center, Tokyo University of Agriculture and Technologyឡ▱┴໭タᴦ㒆ࡢὠල㖔ᒣࡣ㔠㖔ᒣ࡜ࡋ࡚▱ࡽࢀ
1600 ᖺࡇࢁ࠿ࡽ᧯ᴗࢆጞࡵࡓࠋ㔠ࡢ๪⏘≀࡜ࡋ࡚ฟ࡚
ࡃࡿ Sb ࡢ᥇᥀࡜〇㘐ࡶ⾜ࢃࢀ࡚࠸ࡓࠋ㖔ᒣࡣ 1930 ᖺ௦࡟άືࡀ᭱ࡶ┒ࢇ࡛ࠊ1956 ᖺ࡟㛢ᒣࡋࡓ㸯㸧ࠋ⌧ᅾࡣࢫࢠ࡜ࣄࣀ࢟ࡀ᳜ᯘࡉࢀ㐣ཤࡢጼࢆఛ࠺ࡇ࡜ࡣ࡛ࡁ࡞࠸ࠋSb ࡣẘᛶࢆᣢࡘඖ⣲࡜ࡋ࡚▱ࡽࢀ࡚࠾ࡾࠊ▼⏣࡜∦ᒣࡣ⁠㈡┴⡿ཎ⏫࡟࠶ࡿ Sb ࡢ〇㘐ᕤሙ࿘㎶ࡢ Sb ởᰁࢆㄪᰝࡋ࿘㎶ఫẸࡢ೺ᗣ⿕ᐖ࡟ࡘ࠸࡚㆙࿌ࡋࡓ㸰㸧ࠋὠල㖔ᒣ࿘㎶࡟⌧ᅾ࡝ࡢࡃࡽ࠸ Sb ࡀᏑᅾࡍࡿ࠿㐣ཤ࠿ࡽࡢ⤒㐣ࢆࡩࡲ࠼࡚᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࡣ⏘ᴗ⪃ྂᏛⓗほⅬ࠿ࡽࡶ㔜せ࡛࠶ࡿࠋ ᶞᮌࡢᖺ㍯୰࡟ྲྀࡾ㎸ࡲࢀࡓᚤ㔞ඖ⣲ࡸᨺᑕᛶ≀㉁
ࡣ࿘㎶ᅵተࡢ⃰ᗘࢆ཯ᫎࡍࡿࡇ࡜࠿ࡽᶞᮌᖺ㍯ࡈ࡜ࡢ≀㉁㔞ࢆ ᐃࡍࡿࡇ࡜࡛㐣ཤࡢ⎔ቃࡢኚ㑄ࢆゎ࡛᫂ࡁࡿྍ⬟ᛶࢆᣢࡘࠋࡇࡢᶞᮌᖺ㍯ゎᯒἲ࡟ࡼࡾ㖔ᒣ࿘㎶
ࡢ Sb ⃰ᗘࡢኚ㑄ࢆㄪ࡭ࡓࠋSb ࡢᐃ㔞࡟ࡣ㧗ឤᗘ᳨࡛ฟྍ⬟࡞୰ᛶᏊᨺᑕ໬ศᯒἲࢆ⏝࠸ࡓࠋ ୍㒊ࡣࡍ࡛࡟ሗ࿌ࡋ࡚࠸ࡿࡀ 3)ࠊ᪂ࡋࡃ ᐃ⤖ᯝࡶᚓࡽࢀࡓࡢ࡛ຍ࠼࡚ሗ࿌ࡍࡿࠋᐇ㦂ヨᩱὠල㖔ᒣࡢヨᩱ᥇ྲྀᆅⅬࢆ Fig. 1 ࡟♧ࡍ࡜࡜ࡶ࡟ࠊ
Table 1 ࡟ྛᆅⅬࡢ┠༳➼࡜ᶆ㧗ࢆ♧ࡋࡓࠋᅵተヨᩱࡣ
2006 ᖺ࡜ 2007 ᖺ࡟ᆅ⾲࠿ࡽ 10 cm ࡢ῝ࡉ࠿ࡽ᥇ྲྀࡋ
ࡓࠋSb ࡢ᭱኱⃰ᗘࡀ᳨ฟࡉࢀࡓᆅⅬ࡛ Sb ࡢ῝ᗘศᕸࢆぢࡿࡓࡵ 5cm 㛫㝸࡛῝ࡉ 50cm ࡲ࡛ᅵተࢆ᥇ྲྀࡋࡓࠋ
ணഛᐇ㦂࡜㖔ᒣ㊧ᆅࡢ Sb ⃰ᗘࢆẚ㍑ࡍࡿࡓࡵ Sb ࡢởᰁࡣ⪃࠼ࡽࢀ࡞࠸ே㛫⎔ቃ኱Ꮫᵓෆࡢ₇⩦ᯘ࠿ࡽ 2004
࡜ 2005 ᖺ࡟ᅵተࢆ᥇ྲྀࡋࡓࠋ
-557ࣃ࢖ࣉ$⣔⤫ࠉࠉ⎔ቃ⛉Ꮫ

- 366 -

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ᅵተヨᩱࡣ 105Υ࡛ 24 ᫬㛫஝⇱ࡋࡓࠋⲨࡃ○ࡁࠊ

ᆅⅬ㸰࡟㏆࠸ᆅⅬ㸯࡛Sb ࡣ 270 ppm ࡜࡞ࡗࡓࡀࡇࡢ

500 m ࣓ࢵࢩࣗࡢࡩࡿ࠸ࢆ㏻ࡋࡓᚋࠊ㓟໬࢔࣑ࣝࢽ࢘

ᆅⅬࡣ᳃ᯘࡢಖᏲ࡟฼⏝ࡍࡿᯘ㐨ࡢഐ࡛࠶ࡿࠋᚑࡗ࡚

࣒ࡢங㖊࡛⣽࠿ࡃ○࠸ࡓࠋ㖔ᒣ㛢ᒣᚋ᧠஘ࡉࢀࡓࡓࡵᆅⅬ㸰ࡢ್࡟ẚ࡭ప࠸⃰ᗘᶞᮌヨᩱࡣᡂ㛗㗹㸦HagrofSweden AB 〇ࠊ㛗ࡉ 30cmࠊ࡟࡞ࡗࡓ࡜⪃࠼ࡽࢀࡿࠋ

ࢥ࢔ᚄ 5.5mm㸧ࢆ౑⏝ࡋࠊࣄࣀ࢟࡜ࢫࢠᶞᖿ㒊࠿ࡽ 2006ᖺ࡜ 2007 ᖺ࡟᥇ྲྀࡋࡓࠋ᥇ྲྀࡋࡓヨᩱࡣ 105Υ࡛ 24

Sb ࡢ῝ᗘศᕸ

᫬㛫஝⇱ࡋࡓᚋࠊ㎶ᮦ࡜ᚰᮦ࡟ศࡅᙧᡂᒙഃ࠿ࡽࡑࢀ ᅵተ୰ࡢ Sb ࡀ᭱㧗⃰ᗘࢆ♧ࡋࡓᆅⅬ㸰ࡢ࿘㎶ࢆヲࡒࢀ⣙㸳ᖺ㍯ࡈ࡜࡟ษࡾศࡅࡓࠋ

⣽࡟ㄪ࡭ࡓࠋᆅ⾲ࡼࡾ 50 cm ࡢ῝ࡉࡲ࡛᥀ࡾୗࡆ Sb ࡢ ᶞ⓶ヨᩱࡣ 105Υ࡛ 24 ᫬㛫஝⇱ࡋࡓᚋࠊ⣽∦໬ࡋࡓࠋ

⃰ᗘኚ໬ࢆㄪ࡭ࡓࠋ5 cm ้ࡳ࡛ ᐃࡋࡓ Sb ⃰ᗘࢆ Fig.

Sb ࡢᐃ㔞

3 ࡟♧ࡍࠋᆅ⾲㏆ࡃ࡛ 300-390 ppm ࠶ࡗࡓ Sb ࡀ῝ᗘࢆᅵተヨᩱࡣ⣙ 50mg ࠊᶞᮌヨᩱࡣ 300-400mg ࠊᶞ⓶ቑࡍ࡟ࡋࡓࡀ࠸ࡑࡢ⃰ᗘࡣῶᑡࡋࡓࠋࡇࡢ⤖ᯝࡣ㐣ཤ

ࡣ 200mg ࢆ⢭ᶆࡋ࣏࢚ࣜࢳࣞࣥࡢ⿄࡟ධࢀᐦᑒࡋ↷࡟࡞ࢇࡽ࠿ࡢேᕤⓗᙳ㡪ࡀ࠶ࡗࡓࡇ࡜ࢆ♧၀ࡋ࡚࠸ࡿࠋ

ᑕヨᩱ࡜ࡋࡓࠋ୰ᛶᏊ↷ᑕࡣࠊ᪥ᮏཎᏊຊ◊✲㛤Ⓨᶵࡍ࡞ࢃࡕࠊ〇㘐ᕤሙ࠿ࡽ Sb ࡀ㣕ᩓࡋᆅ⾲࡟㞟✚ࡋ࡚⌧

13

ᵓࡢ JRR-4 ࡢ㹒ࣃ࢖ࣉ㸿⣔⤫㸦୰ᛶᏊ᮰ 5.3 x 10
-2122cm )࡛ 20 ࡞࠸ࡋ 30 ศ㛫⾜ࡗࡓࠋ Sb ࡜nᅾࡶࡑࡢᙳ㡪ࡀṧࡗ࡚࠸ࡿ࡜᥎ ࡛ࡁࡿࠋ124

Sb ࡢȚ⥺

ᐃࡣࠊ↷ᑕ⣙㸵᪥ᚋ࠿ࡽ 7,000 ⛊㛫⾜ࡗࡓࠋ
Sb ࡢᐃ㔞ࡣࠊཎᏊ྾ගศᯒ⏝ᶆ‽ヨᩱࢆࢁ⣬ୖ࡟୍ᐃ㔞⁲ୗࡋ஝⇱ࡋࡓࡢࡕࠊ࣏࢚ࣜࢳࣞࣥࢩ࣮ࢺ࡛ᐦᑒ
ࡋヨᩱ࡜ྠࡌࡼ࠺࡟↷ᑕࡋ࡚ヨᩱࡢȚ⥺࡜ẚ㍑ࡋࡓࠋ⤖ᯝ࡜⪃ᐹᅵተ୰ࡢ㹑㹠⃰ᗘ㖔ᒣ㊧ᆅࡢ㹑㹠⃰ᗘศᕸὠල㖔ᒣ㊧ᆅࡢᅵተ୰ࡢ Sb ⃰ᗘࢆ Fig. 2 ࡟♧ࡍࠋSb⃰ᗘࡣ᥇ྲྀሙᡤ࡟ࡼࡾ 8 ppm ࠿ࡽ 17,000ppm ࡜኱ࡁࡃ␗࡞ࡗࡓࠋ᥇ྲྀᆅⅬ㸰࡛᭱኱್ࢆ♧ࡋᩳ㠃ࡢ㡬ୖ࡟㏆࡙ࡃ࡟ࡋࡓࡀ࠸ࠊࡑࡢ⃰ᗘࡣῶᑡࡋࡓࠋᆅⅬ㸶ࡢ್ࢆ㝖ࡁឡ▱┴ᒸᓮᕷᮏᒣ⏫࡟࠶ࡿே㛫⎔ቃ኱Ꮫ₇⩦ᯘࡢᅵተ୰ࡢ Sb ⃰ᗘ㸦1 – 2 ppm㸧ࡼࡾ㧗࠸್࡜࡞ࡗࡓࠋSb࡛ởᰁࡉࢀ࡚࠸࡞࠸ᅵተࡢ Sb ⃰ᗘࡣᩥ⊩್࡛ 0.2 – 2

3-13

ppm ࡜ሗ࿌ࡉࢀ࡚࠸ࡿ 4)ࠋ

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᥇ྲྀᆅⅬ㸰࿘㎶ࡢ Sb ศᕸᶞᮌᖺ㍯୰ࡢ Sb ศᕸ࡜ᶞ⓶ࡢ Sb ⃰ᗘ ᥇ྲྀᆅⅬ㸰ࢆ୰ᚰ࡟ࡋ࡚すࠊ໭ࠊ༡す᪉ྥ࡟ 10 m 㛫

ࣄࣀ࢟ᖺ㍯୰ࡢ Sb ศᕸ㝸࡛ᅵተヨᩱࢆ᥇ྲྀࡋࡓࠋ⤖ᯝࢆ Table㸰࡟♧ࡍࠋ ␗࡞ࡿ㸳ᆅⅬ࡛⏕⫱ࡋࡓࣄࣀ࢟ᖺ㍯୰ࡢ Sb ศᕸࢆすഃ᪉ྥ࡟ἢࡗ࡚ Sb ⃰ᗘࡀ㧗⃰ᗘ࡟࡞ࡗࡓࠋࡇࡢ

Fig. 4 ࡟♧ࡍࠋྛ␒ྕࡣᅵተࢆ᥇ྲྀࡋࡓᆅⅬࡢ␒ྕ࡟ᑐ

ᐃᆅⅬࡢ࿘㎶࡟ࡣᆅⅬ㸰࡜ྠᵝ࡞ᕤሙࡢṧ㧁ࡀṧࡗ࡚ᛂࡋ࡚࠸ࡿࠋ
Sb ⃰ᗘࡣ᭱ࡶእഃࡢᖺ㍯࡛᭱኱್ࢆ♧ࡋࠊ࠸ࡓࠋࡇࡢሙᡤ࡛ࡶ〇㘐ࡢᙳ㡪ࢆཷࡅࡓࡶࡢ࡜ᛮࢃࢀ

㎶ᚰᮦቃ⏺࡟ྥࡅῶᑡࡋࡓࡢࡕᚰᮦ㒊࡛࡯ࡰ୍ᐃ್࡜

ࡿࠋ࡞ࡗࡓࠋᅵተヨᩱࡢ Sb ⃰ᗘࡀ᭱ࡶ㧗࠿ࡗࡓᆅⅬ㸰࡛⏕⫱ࡋࡓࣄࣀ࢟ࡢ Sb ศᕸࡣ௚ࡢ᭤⥺࡜ఝࡓࣃࢱ࣮ࣥࡀ
ᚓࡽࢀࡓࡀࠊSb ⃰ᗘࡣ඲యⓗ࡟㧗ࡃ௚ࡢヨᩱ࡜ẚ࡭㸳ಸ⛬ᗘࡢ್࡜࡞ࡗࡓࠋ

3-13- 368 -

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ࢫࢠᖺ㍯୰ࡢ Sb ศᕸࡇࢀࡽࡢ⤖ᯝࢆ⥲ྜࡍࡿ࡜ࠊࡇࡢᖺ㍯ゎᯒἲ࡛ὠල㖔 Figure 5 ࡟㸱ᮏࡢࢫࢠᖺ㍯୰ࡢ Sb ศᕸࢆ♧ࡍࠋ␒ྕᒣ㊧ࡢ㐣ཤࡢ Sb ⎔ቃኚືࢆホ౯ࡍࡿࡇ࡜ࡣᅔ㞴࡛࠶ࡣࣄࣀ࢟࡜ྠᵝᅵተ᥇ྲྀᆅⅬࡢ␒ྕ࡟ᑐᛂࡋ࡚࠸ࡿࠋ

ࡿࡇ࡜ࡀศ࠿ࡗࡓࠋ

㸱ᶞᮌᖺ㍯ࡢศᕸ᭤⥺ࡢࣃࢱ࣮ࣥࡣࡑࢀࡒࢀ␗࡞ࡾࠊ
ࣄࣀ࢟ࡢࡑࢀ࡜ࡶ␗࡞ࡗࡓࠋᆅⅬ㸰ࡢヨᩱ࡛ࡣࣄࣀ࢟
࡜ྠᵝ Sb ⃰ᗘࡀ௚ࡢヨᩱ࡟ẚ࡭඲యⓗ࡟㧗࠸್࡜࡞
ࡗࡓࠋ

3-13

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ࣄࣀ࢟࠾ࡼࡧࢫࢠᶞ⓶୰ࡢ Sb

Around the Abandoned Tsugu Mine in Aichi Prefecture by ࣄࣀ࢟࠾ࡼࡧࢫࢠᶞ⓶୰ࡢ Sb ⃰ᗘࢆ Table 3 ࡟♧ࡍࠋ

Neutron Activation Analysis, Journal of Radiochemical andᆅⅬ㸰࡜ᆅⅬ㸱࡟⏕⫱ࡍࡿᶞ⓶୰ࡢ Sb ⃰ᗘࡣ௚ࡢᆅ

Nuclear chemistry, 278 (2008) 283

Ⅼ࡛ᚓࡓᶞ⓶୰ࡢ⃰ᗘ࡟ẚ࡭㧗࠸್ࢆ♧ࡋࡓࠋࡇࡢ⤖4. ὸぢ㍤ኵ㸸᪥ᮏᅵተࡢ᭷ᐖ㔠ᒓởᰁࠊ࢔ࢢࢿᢏ⾡ࢭᯝࡣᶞᮌࡀ⏕⫱ࡍࡿᅵተ⎔ቃࢆ཯ᫎࡋ࡚࠸ࡿ࡜ぢ࡞ࡍࣥࢱ࣮ (2001)263.

ࡇ࡜ࡀ࡛ࡁࡿࠋࡍ࡞ࢃࡕᶞ⓶ࡣࣂ࢖࢜ࣔࢽࢱ࣮࡜ࡋ࡚
ࡢྍ⬟ᛶࡀ࠶ࡿࠋ

ᡂᯝࡢබ⾲
Y. Katayama, A. Misawa, N. Yamada, S. Yachi, H. Muto, T.
Aoki, Y. Kawabata, and M. Nagai, Analysis of Antimony
Around the Abandoned Tsugu Mine in Aichi Prefecture by
Neutron Activation Analysis, Journal of Radiochemical andNuclear chemistry, 278 (2008) 283

3-13⤖ㄽ
ὠල㖔ᒣ㊧ᆅࡢ㸶ᆅⅬࡢᅵተ୰ Sb ⃰ᗘࡣ 8 - 17,000
ppm ࡜࡞ࡗࡓࠋ〇㘐ᕤሙࡢᇶ♏㒊ศ࡜ᛮࢃࢀࡿṧ㧁ࡀṧࡗ࡚࠸ࡿᆅⅬ㸰ࡢ⾲ᒙᅵተ୰ࡢ Sb ࡣࠊ17,000ppm ࡜ᴟࡵ࡚㧗࠸್ࢆ♧ࡋ῝ࡉ࡜࡜ࡶ࡟ῶᑡࡋࡓࠋࡇࡢࡇ࡜
ࡣ㐣ཤ࡟〇㘐ᕤሙࡀᏑᅾࡋ᧯ᴗࡋ࡚࠸ࡓࡇ࡜ࢆ᫂ࡽ࠿
࡟ࡍࡿࡶࡢ࡛࠶ࡿࠋࡇࡢࡼ࠺࡟〇㘐ᕤሙ࿘㎶ᅵተ୰ࡢ
Sb ⃰ᗘࡀ㧗࠸ࡇ࡜࠿ࡽ᧯ᴗᙜ᫬〇㘐సᴗ࡟ᚑ஦ࡋࡓ⪅ࡢ࡞࠿࡟ࡣከ㔞ࡢ Sb ࡟ࡉࡽࡉࢀࡓ⪅ࡀ࠸ࡓ࡜᥎ᐹࡉ
ࢀࡿࠋ⌧ᅾࡶ Sb ࡢởᰁ࡟ὀពࡀᚲせ࡛࠶ࡿࠋ ࡲࡓࠊSb ࡣࣄࣀ࢟ࡸࢫࢠ࡟ྲྀࡾ㎸ࡲࢀ࡟ࡃࡃ㧗ឤᗘࡢᨺᑕ໬ศᯒἲ࡛ᐃ㔞ࡋࡓ࡟ࡶ࠿࠿ࢃࡽࡎ᳨ฟ㝈⏺࡟㏆ࡃ᫂░࡞ഴྥࡣᚓࡽࢀ࡞࠿ࡗࡓࠋࡇࡢ⤖ᯝ࠿ࡽᖺ㍯
ゎᯒἲ࡛ὠල㖔ᒣࡢ Sb ⎔ቃࢆ㐣ཤ࡟㐳ࡗ࡚᥎ᐃࡍࡿ
ࡇ࡜ࡣᅔ㞴࡛࠶ࡿࡇ࡜ࡀศ࠿ࡗࡓࠋ
ㅰ㎡ᨺᑕ໬ศᯒ࡟㛵ࡍࡿᣦᑟຓゝࢆ㡬ࡁࠊࡲࡓ ᐃ࡟ࡈຓຊ࠸ࡓࡔ࠸ࡓᮾி኱Ꮫ኱Ꮫ㝔ᕤᏛ⣔◊✲⛉ཎᏊຊᑓᨷඹྠ฼⏝⟶⌮ᮏ㒊㸦኱Ꮫ㛤ᨺ◊✲ᐊ㸧ࡢࢫࢱࢵࣇࡢ
᪉ࠎ࡟ឤㅰࡢពࢆ⾲ࡋࡲࡍࠋᩥ⊩
1. ⸨ᇛ㇏㸸 ὠල㔠ᒣࠊ⚾ᮏ(1982)
2. ▼⏣⣖㑻ࠊ∦ᒣᖾኈ㸸࢔ࣥࢳࣔࣥ࡟ࡼࡿ⎔ቃởᰁࠊ⛉Ꮫࠊ48 (1978) 509
3. Y. Katayama, A. Misawa, N. Yamada, S. Yachi, H. Muto,
T. Aoki, Y. Kawabata, and M. Nagai: Analysis of Antimony- 370 -

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JAEA-Review 2013-039


3-14ࢧࣥࢦ㦵᱁୰ࡢࣁࣟࢤࣥඖ⣲ࡢᨺᑕ໬ศᯒ,QVWUXPHQWDO1HXWURQ$FWLYDWLRQ$QDO\VLVRI+DORJHQLQ&RUDO6NHOHWRQV኱ฟ ⱱࠊ⏣୰೺ኴ㑻
62KGH.7DQDND
⌰⌫኱Ꮫ⌮Ꮫ㒊)DFXOW\RI6FLHQFH8QLYHUVLW\RIWKH5\XN\XV ࡣࡌࡵ࡟

ᨺᑕ໬ศᯒࢆ 31 Ẽ㏦⟶↷ᑕࠊ࣐࢞ࣥ⥺ ᐃ⿦ ࢧࣥࢦ㦵᱁㸦⤖ᬗᙧ㸸࢔ࣛࢦࢼ࢖ࢺࠊ୺ᡂศ㸸⨨ࢆ౑ࡗ࡚⾜ࡗࡓࠋᮏ◊✲࡛ࡣࠊヨᩱ࡜ࡋ࡚ࡣࠊ

&D&2㸧୰ࡢ࡛ࡁࡿࡔࡅከࡃࡢඖ⣲ศᯒ࠿ࡽࠊࢧ

Ἀ⦖ࠊ࿴ḷᒣࠊࢱ࢖ࠊ࣏ࢼ࣌ࠊࣇ࢕ࣜࣆࣥࡢࢧࣥ

ࣥࢦࡀ⏕⫱ࡋ࡚࠸ࡓ⎔ቃỈ࡟ࡘ࠸࡚ࡢ᝟ሗࢆᚓ

ࢦ♋࡛᥇ྲྀࡋࡓࢧࣥࢦ㦵᱁ࡢࣇࢵ⣲ࡢᨺᑕ໬ศ

ࡿࡇ࡜ࡀᮏ◊✲ࡢ┠ⓗ࡛࠶ࡿࠋࢧࣥࢦ㦵᱁࡬ࡢ㝜ᯒࢆ࠾ࡶ࡟⾜ࡗࡓࠋ࢖࢜ࣥඹỿᶵᵓࢆゎ᫂ࡍࡿࡇ࡜࡟ࡼࡗ࡚ࠊࢧࣥࢦ

ࡀ⏕⫱ࡋ࡚࠸ࡓ⎔ቃỈࡢ᝟ሗࢆᚓࡿࡇ࡜ࡀྍ⬟ ࢧࣥࢦヨᩱ࡛࠶ࡿࠋ ౯㝜࢖࢜ࣥࡢ &D&2 ࡬ࡢඹỿࡀࠊࡘࡂ

 Ⅳ㓟ሷᶆ‽࡜ࡋ࡚ᆅ㉁ㄪᰝᡤࡀసᡂࡋࡓ

ࡢ࢖࢜ࣥ஺᥮࡛㉳ࡇࡿ࡜௬ᐃࡍࡿ࡜ࠊ&D&2$-&S ࢧࣥࢦ ࠊ-'R㸦ࢻ࣐ࣟ࢖ࢺ㸧ࢆ౑⏝ࡋࡓࠋ

&D$&2㸦$ࡣ  ౯㝜࢖࢜ࣥ㸧ࠊࡑࡢᖹ⾮ᐃࢧࣥࢦ㦵᱁ヨᩱࡣἈ⦖㸦ࣝ࢝ࣥ♋ࠊỈ㔩㸧ࠊሜ㸦࿴




 

ᩘࡣࠊ. >&D$@>&2 @>&D&2@>$ @ ࡜᭩ࡅࡿࠋ

ḷᒣ㸧ࠊࢱ࢖㸦࢝ࣥ࢝࢜ᓥ㸧ࠊࣇ࢕ࣜࣆࣥ㸦ࢭࣈࡑࡋ࡚ࠊ>&D$@>&D&2@ .>$@>&2@࡜ኚᙧ࡛ᓥ㸧ࠊ࣏ࢼ࣌ࡢࢧࣥࢦ♋࠿ࡽ᥇ྲྀࡋࠊ࣑ࣜ࢟ࣗ࢘

ࡁࡿࠋࡋࡓࡀࡗ࡚ࠊࢧࣥࢦ㦵᱁୰ࡢ㝜࢖࢜ࣥྵ㔞Ỉ࡛ᩘᅇࠊ㉸㡢ἼὙίࡋࠊ஝⇱ࡋ࡚‽ഛࡋࡓࠋ

ࡣࠊࢧࣥࢦࡀ⏕⫱ࡋࡓᾏỈࡢⅣ㓟࢖࢜ࣥ࡜㝜࢖࢜ࣥࡢẚ࡟ࡼࡗ࡚Ỵᐃࡉࢀࡿྍ⬟ᛶࡀ࠶ࡿ㸦ࢧࣥࢦ ࣁࣟࢤࣥࡢᨺᑕ໬ศᯒ

ࡢ㓟୙⁐ゎ㒊ࡣ 㸣௨ୗ࡛࠶ࡾࠊ࢖࢜ࣥ஺᥮ࢆ ࢧࣥࢦࡣ୺ᡂศࡀⅣ㓟࢝ࣝࢩ࣒࢘ ⣙  ࡛࠶௬ᐃࡍࡿࡇ࡜ࡣྍ⬟࡛࠶ࡿ㸧ࠋ࢔ࣛࢦࢼ࢖ࢺ⤖ᬗࡾࠊ&D ࠾ࡼࡧ &D ࢆෆ㒊ᶆ‽࡜ࡋ࡚ࡋ࡚౑⏝ࡋࠊ࡬ࣇࢵ໬≀࢖࢜ࣥ㸦)㸧 ಶࡀⅣ㓟࢖࢜ࣥ  ಶࡢḟࡢ↷ᑕࠊ ᐃ᮲௳࡟ࡼࡗ࡚㠀◚ቯᨺᑕ໬ศᯒࢆ

ࢧ࢖ࢺ࡬⨨᥮ࡍࡿྍ⬟ᛶࡣ࠶ࡿࠋࡋ࠿ࡋࠊሷ໬≀⾜ࡗࡓࠋ31 -550 ↷ᑕࢧࣥࢦ୰ࡢࣇࢵ⣲ࢆ࢖࢜ࣥࡼࡾ኱ࡁ࠸ࣁࣟࢤࣥࡣࣇࢵ໬≀࢖࢜ࣥࡼ࠾ࡶ࡟ᐃ㔞ࡍࡿࡓࡵ࡟ࠊࢧࣥࢦヨᩱ㸦⢊ᮎࡲࡓࡣࡾ࢖༙࢜ࣥᚄࡀ኱ࡁ࠸ࡢ࡛ࠊⅣ㓟࢖࢜ࣥ  ಶ࡟ᑐࣈࣟࢵࢡ≧㸧PJ ࢆ࣏ࣜ⿄࡟ᑒධࠊ㧗⣧ᗘ࣏ࡋ࡚  ಶࡢ⨨᥮ࡣࡴࡎ࠿ࡋ࠸࠿ࡶࡋࢀ࡞࠸ࠋࡑࡇ

࢚ࣜࢳࣞࣥ↷ᑕ⏝࢟ࣕࣉࢭࣝ࡟  ヨᩱධࢀࠊ31࡛ࠊࢧࣥࢦ㦵᱁୰ࡢࣁࣟࢤࣥඖ⣲ࢆᐃ㔞ࡍࡿព⩏

Ẽ㏦⟶࡛  ⛊↷ᑕࠊ ⛊㛫ࡢ෭༷᫬㛫ࢆ࠾ࡁࠊࡀ࠶ࡿࠋᖹᡂ㸯㸶ᖺᗘ࠿ࡽ㸰㸮ᖺᗘࡲ࡛ࡢ  ᖺ㛫ࠊ࢟ࣕࣉࢭࣝࢆ㛤ᑒࡋ࡞࠸࡛ࠊ࣐࢞ࣥ⥺ࢫ࣌ࢡࢺࣟ

-55 ཎᏊ⅔ࢆ౑ࡗ࡚ࢧࣥࢦヨᩱ୰ࡢࣁࣟࢤࣥࡢ

࣓࣮ࢱ࣮ࢆ⏝࠸࡚  ⛊㛫 ᐃࢆ⾜࠸ࠊ)



)

㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝◊✲᪋タ࡜⿦⨨                  ◊✲ศ㔝
-55 31ࠊẼ㏦⟶   ⎔ቃ໬Ꮫࠊᾏὒᆅ⌫໬Ꮫ- 371 -

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JAEA-Review 2013-039

NH9 ࡜ $O $ONH9 ࢆᐃ㔞ࡋࡓࠋᶆୖᘧࡣࠊᾏỈࡢࣇࢵ໬≀࢖࢜ࣥ࡜Ⅳ㓟࢖࢜ࣥࡢ‽ࡣࣇࢵ໬࢝ࣝࢩ࣒࢘ࢆⅣ㓟࢝ࣝࢩ࣒࢘࡟ΰྜ

ẚࡀࠊⅣ㓟ሷ࡟ඹỿࡍࡿࣇࢵ໬≀࢖࢜ࣥ㔞ࢆࢥࣥࡉࡏ࡚సᡂࡋࡓࠋࡉࡽ࡟ࠊ ศࡢ෭༷᫬㛫ࢆࢺ࣮ࣟࣝࡍࡿࡇ࡜ࢆ♧ࡋ࡚࠸ࡿࠋࡉࡽ࡟ࠊᾏỈࡢ࠾ࡁࠊ ศ㛫 ᐃࢆ⾜࠸ࠊ1Dࠊ&Oࠊ0Qࠊ6Uࠊ, ࡀⅣ㓟࢖࢜ࣥࡣࠊS+ ࡜㛵ಀࡍࡿࠋࡋࡓࡀࡗ࡚ࠊᾏ

ศᯒྍ⬟࡛࠶ࡗࡓࠋ

Ỉࡢ S+ ࠾ࡼࡧ஧㓟໬Ⅳ⣲࡟㛵ࡍࡿ᝟ሗࡀᚓࡽࢀ

ࡿྍ⬟ᛶࡀ࠶ࡿࠋࡑࡇ࡛ࠊࢧࣥࢦẆࡢࣇࢵ⣲ࡢṇ ⤖ᯝ࡜⪃ᐹ☜࡞ᐃ㔞ࡀ㔜せ࡛࠶ࡿࠋࡑࡇ࡛ࠊ࿴ḷᒣ㸦ሜ㸧ἈⅣ㓟ሷᶆ‽㸦-&Sࠊ-'R㸧ࢆࢧࣥࢦࡢᨺᑕ໬

⦖㸦ࣝ࢝ࣥ♋ࠊỈ㔩㸧ࠊࢱ࢖㸦࢝ࣥ࢝࢜ᓥ㸧ࠊࣇศᯒࡢẚ㍑ᶆ‽࡜ࡋ࡚౑⏝ࡍࡿࡇ࡜ࡀྍ⬟࠿ࢆ࢕ࣜࣆࣥ㸦ࢭࣈᓥ㸧㸪࣏ࢼ࣌ᓥࡢࢧࣥࢦ♋࠿ࡽ᥇᳨ウࡍࡿ┠ⓗ࡛ࠊᶆ‽ヨᩱࡢศᯒࢆ⾲  ࡟♧ࡍࡼྲྀࡋࠊ‽ഛࡋࡓࢧࣥࢦ㦵᱁ヨᩱࡢᨺᑕ໬ศᯒࢆ⾜࠺࡟  ᅇ௨ୖ⧞ࡾ᭰࠼ࡋᨺᑕ໬ศᯒࡋࡓࠋ-&Sࠊࡗࡓ⤖ᯝࢆ⾲  ࡟♧ࡍࠋ

-'R ࡢࣇࢵ⣲ศᯒ್ࡣࡑࢀࡒࢀࠊSSPࠊ ࢧࣥࢦ㦵᱁ࡢࣇࢵ⣲ྵ㔞࡜ࢧࣥࢦࡀᡂ⫱ࡋࡓ

SSP ࡛࠶ࡿ㸦⾲ 㸧ࠋࡲࡓࠊᨺᑕ໬ศᯒࡢಙ㢗ᛶ

ᾏᇦࡢⅣ㓟࢖࢜ࣥ⃰ᗘࡢ㛵ಀࢆ⪃ᐹࡍࡿࡓࡵ࡟ࠊ
ࢆࢳ࢙ࢵࢡࡍࡿ┠ⓗ࡛ࠊヨᩱࢆ㝧࢖࢜ࣥ஺᥮ᶞ⬡ࢧࣥࢦࢆ᥇ྲྀࡋࡓᾏᇦࡢⅣ㓟࢖࢜ࣥ⃰ᗘࢆ௨ୗࢆ౑ࡗ࡚⁐ゎࡋࠊࣇࢵ໬≀࢖࢜ࣥࢆ࢖࢜ࣥࢡ࣐ࣟ

ࡢ᪉ἲ࡛ィ⟬ࡍࡿࡇ࡜ࡀྍ⬟࡛࠶ࡿࠋሷศࠊ࢔ࣝ

ࢺἲࢆ౑ࡗ࡚ศᯒࡋࡓࠋࡉࡽ࡟ࠊヨᩱࢆᕼሷ㓟࡟࢝ࣜᗘࠊS&2 ࡢ್ࢆ୍ᐃ㸦ሷศSVX࢔ࣝ࢝ࣜ

⁐ゎᚋࠊ࢔ࣝࣇࢵࢯࣥࢆࡘ࠿ࡗ࡚ⓎⰍࡉࡏࠊࣇࢵ

ᗘPPRONJS&2 ȣDWP㸧࡜ࡋ࡚ࠊᾏ

⣲ࢆẚⰍศᯒἲ࡟ࡼࡗ࡚ᐃ㔞ࡋࡓࠋ⾲  ࡟ࡑࡢ⤖Ỉࡢ ᗘࢆ Υ࠿ࡽ Υࡲ࡛ Υẖ࡟ኚ໬ࡉᯝࢆࡲ࡜ࡵࡓࠋ໬Ꮫศ㞳᧯సࢆక࠺ศᯒἲࢆ౑ࡗ

ࡏࠊ኱Ẽ஧㓟໬Ⅳ⣲㸦SSP㸧ࡀ  Ẽᅽୗ࡛ᾏࡓࣇࢵ⣲ࡢศᯒࢹ࣮ࢱࡣᨺᑕ໬ศᯒ࡟ࡼࡗ࡚ᚓ

Ỉ࡜໬Ꮫᖹ⾮࡟࠶ࡿ࡜௬ᐃࡋࠊᾏỈ୰ࡢⅣ㓟࢖࢜ࡽࢀࡓࢹ࣮ࢱ࡜ẚ㍑ࡋ࡚ᑡࡋᑠࡉ࡞್ࢆ♧ࡋࡓࠋࣥ⃰ᗘࡀィ⟬࡛ࡁࡿࠋᾏỈ୰ࡢⅣ㓟࢖࢜ࣥ⃰ᗘࡣ

-&S ࡣࠊ▼ᇉᓥ࠿ࡽ᥇ྲྀࡋࡓࣁ࣐ࢧࣥࢦ࠿ࡽసᾏỈ ࡢୖ᪼࡜࡜ࡶ࡟ቑຍࡍࡿഴྥࡀ࠶ࡿࠋᾏỈᡂࡉࢀ࡚࠸ࡿࡢ࡛ࠊࢧࣥࢦࡢࣇࢵ⣲ศᯒ⏝ࡢᶆ‽୰ࡢࣇࢵ໬≀࢖࢜ࣥࡣಖᏑᛶᡂศ࡛࠶ࡿࡢ࡛ࠊࡑ≀㉁࡜ࡋ࡚᭱㐺࡛࠶ࡿ࡜ᛮࢃࢀࡿࠋࡋ࠿ࡋࠊ⾲ ࡢ⃰ᗘࡣሷศ SVX ࡟ᑐࡋ ȣ0 ࡛࠶ࡿࠋࡼࡗ

࡟♧ࡋࡓࡼ࠺࡟ࠊ-&S ୰ࡢࣇࢵ⣲ྵ㔞ࢆṇ☜࡟࡚ࠊ>)@㸦DT㸧>&2@㸦DT㸧ࡣ ᗘࡢୖ᪼࡟క࠸ῶ

Ỵᐃࡍࡿࡲ࡛࡟ࡣᮏ◊✲࡛ࡣ⮳ࡽ࡞࠿ࡗࡓࠋ௒ᚋࠊ

ᑡࡍࡿࠋ⏕⫱ᾏᇦࡢᾏỈ ࡀ㧗࠸࡯࡝ࠊᾏỈ୰ࡢศᯒᅇᩘࢆቑࡸࡍ࡞࡝ࡋ࡚ࠊಙ㢗ᛶࡢ㧗࠸ࢹ࣮ࢱⅣ㓟࢖࢜ࣥ࡜ࣇࢵ໬≀࢖࢜ࣥࡢ⃰ᗘẚࡀᑠࡉࡃࢆᚓࡿࡇ࡜࡟ࡼࡗ࡚ࠊ-&S ࢆᨺᑕ໬ศᯒࡢᶆ‽࡞ࡿࠋࡋࡓࡀࡗ࡚ࠊୖᘧ࠿ࡽࢧࣥࢦࡢ⏕⫱ᾏỈࡢヨᩱ࡜ࡍࡿࡼ࠺࡟ࡋࡓ࠸ࠋ

ᗘࡀ㧗࠸࡯࡝ࢧࣥࢦ㦵᱁୰ࡢࣇࢵ⣲ྵ㔞ࡀᑠᮏ◊✲࡛ࡣࠊ
≉࡟ࠊࢧࣥࢦ୰ࡢࣇࢵ⣲ྵ㔞࠿ࡽࠊࡉࡃ࡞ࡿഴྥࡀண ࡉࢀࡿࠋࢧࣥࢦ㦵᱁ࡢᡂ㛗⋡ࢧࣥࢦࡀ⏕ᜥࡋ࡚࠸ࡓ⎔ቃỈࡢ໬Ꮫ⤌ᡂࢆ᥎ᐃࡣ࠾ࡼࡑ FP\U ࡞ࡢ࡛ヨᩱ࡟⏝࠸ࡓ㦵᱁ࡀᙧࡍࡿࡇ࡜ࢆヨࡳࡓࠋᾏỈ࠿ࡽ࢔ࣛࢦࢼ࢖ࢺ࡬ࡢ

ᡂࡉࢀࡓࡢࡣ᥇ྲྀ௨๓ࡢ⣙  ᖺ㛫࡛࠶ࡿࠋ᥇ྲྀᆅ

ࣇࢵ໬≀࢖࢜ࣥࡢඹỿࡣḟࡢ࢖࢜ࣥ஺᥮཯ᛂᘧ

ࡈ࡜࡟ࡇࡢᮇ㛫ࡢ  ࣨ᭶ẖࡢᖹᆒᾏỈ ࢆ࢔࣓࡛㉳ࡇࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ ,FKLNXQL ࠋࣜ࢝ᾏὒ኱Ẽᒁ㸦KWWSZZZQRDDJRYZ[KWPO㸧






&D&2 V ) DT  &D) V &2
 .) >&D)@>&2@>&D&2@>)@DT 

ࡢேᕤ⾨࡛ᫍほ ࡋࡓ⾲㠃ᾏỈࡢ ᗘࡢࢹ࣮ࢱ
ࢆ⏝࠸࡚ࠊ⏕⫱ᮇ㛫ࡢᖺᖹᆒᾏỈ ࡜ᾏỈࡢⅣ㓟

3-14- 372 -

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JAEA-Review 2013-039

࢖࢜ࣥ⃰ᗘࢆィ⟬ࡋࠊ⾲  ཬࡧᅗ  ࡟♧ࡍࠋࢧࢆẚ㍑᳨ウࡋࠊࢧࣥࢦࡀ⏕ᜥࡋ࡚࠸ࡓ⎔ቃỈࡢࣥࢦࡀ⏕⫱ࡋࡓᾏỈࡢ ᗘࡀప࠸࡯࡝㦵᱁୰ࡢ໬Ꮫ⤌ᡂ࡜ࡢ㛵ಀࢆ⪃ᐹࡍࡿணᐃ࡛࠶ࡿࠋ

ࣇࢵ⣲ྵ㔞ࡀ኱ࡁ࠸ྍ⬟ᛶࡀ࠶ࡾ⾲  ࡢ ᗘࢹ࣮ࢱ࠿ࡽ࣏ࢼ࣌࢝ࣥ࢝࢜ࢭࣈỈ㔩ࣝ࢝ࣥ

ࠊᘬ⏝ᩥ⊩♋ሜ ࡢࢧࣥࢦヨᩱࡢ㡰࡟ࣇࢵ⣲ྵ㔞ࡀ኱ࡁ(1) Aizawa S., AkaiwaH. Bull. Chem. Soc. Japan,
68(1995)825

ࡃ࡞ࡿࡇ࡜ࡀண᝿ࡉࢀࡿ⾲  ࡟ࡲ࡜ࡵࡓࣇࢵ⣲ྵ㔞ࡢᖹᆒ್ࡣ࣏ࢼ࣌࡜࢝ࣥ࢝࢜ࡢ㡰ࡀ࠸ࢀ(2) Ando A. et al., Bull. Geol. Surv. Japan,41(1990)27

࠿ࢃࡗ࡚࠸ࡿ௨እࡣࢭࣈỈ㔩ࣝ࢝ࣥ♋ሜ(3) Ichikuni M. Chem. Geol. 27(1979)207.

ࡢ㡰࡟኱ࡁ࡞್ࢆ♧ࡋ࡯ࡰண᝿࡝࠾ࡾ࡛࠶

(4) Ichikuni M., Tsurumi M., Anal. Sci., 6(1990) 111(5) Ramos A. A. et al., J. Radioanal. Nucl. Chem.,ࡿ257(2003)441

ࢧࣥࢦ㦵᱁࡟ඹỿࡋࡓࣇࢵ⣲ྵ㔞ࢆ ᐃࡋࣇࢵ⣲ྵ㔞࡜ࢧࣥࢦࡀ⏕⫱ࡋࡓᾏᇦࡢⅣ㓟࢖࢜ࣥ⃰ᗘࡢ㛵ಀࢆ⪃ᐹࡋࡓࠋࡑࡢ⤖ᯝࠊࢧࣥࢦ㦵᱁ࠊᡂᯝࡢබ⾲ࡢࣇࢵ⣲ྵ㔞ࡣᾏỈ୰ࡢⅣ㓟࢖࢜ࣥ⃰ᗘ࡟཯ẚ(1) ኱ฟⱱࠊྜྷᮧ࿴ஂ㸦2006㸧ࠕⅣ㓟ሷࡢᆅ⌫໬Ꮫࠖ࡟ࡼࡏ࡚ࠊᆅ⌫໬Ꮫࠊ40㸪177-178

౛ࡍࡿഴྥࢆ♧ࡋࡓ㸦ᅗ 㸧ࠋࡲࡓᾏỈ࡜኱Ẽ㛫ࡢ஧㓟໬Ⅳ⣲ᖹ⾮ࢆ௬ᐃࡋࡓィ⟬ࡢ⤖ᯝࠊᾏỈ
୰ࡢⅣ㓟࢖࢜ࣥ⃰ᗘࡣᾏỈࡢ ᗘࡢ⣼஌࡟ẚ౛(2) ⏣୰೺ኴ㑻,኱ฟⱱ㸦2007㸧ࢧࣥࢦ㦵᱁୰ࡢࣇࢵ⣲ྵ㔞࡜ᾏỈ୰ࡢⅣ㓟࢖࢜ࣥ⃰ᗘࡢ㛵ಀ, ᪥ᮏᾏỈᏛ఍ㄅ, 61, 118-122

ࡋ࡚ኚືࡍࡿ࡜ィ⟬࡛ࡁࡿࠋ
(3) ኱ฟⱱ㸦2007㸧ࢧࣥࢦࡢ໬Ꮫീࢆ㏻ࡋ࡚ࡳࡿ
ᾏὒ⎔ቃࡢኚ㑄, ᾏὒ໬Ꮫ◊✲, 20, 54-77

ࠊ௒ᚋࡢ᪉㔪ᮏ◊✲ࡣࠊ࠾ࡶ࡟ࣇࢵ⣲ࡢᨺᑕ໬ศᯒ࡟ࡘ࠸
࡚⾜ࢃࢀࡓࠋࣇࢵ⣲ࠊሷ⣲ࠊ⮯⣲ࠊࣚ࢘⣲࡞࡝ࣁࣟࢤࣥඖ⣲ࡢᚤ㔞ศᯒ࡟㛵ࡋ࡚ᐇ⏝ⓗ࡛᭱㐺࡞ᶵჾศᯒἲࡣ☜❧ࡋ࡚࠸ࡿ࡜ࡣゝ࠼࡞࠸ࠋࡇ
ࡇ࡛♧ࡋࡓࡼ࠺࡟ᨺᑕ໬ศᯒࡣࡑࢀࡽࡢඖ⣲ࡢ౽฼࡞ศᯒἲࡢ  ࡘ࡛࠶ࡿࠋࡲࡓࠊ㝧࢖࢜ࣥඖ⣲ࡸ㑄⛣ඖ⣲࡟㛵ࡋ࡚ࡣࠊ⌰⌫኱Ꮫ࡟タ⨨ࡉࢀ࡚࠸ࡿ ,&306 ࢆ౑ࡗ࡚ࠊᨺᑕ໬ศᯒࢆ࠾ࡇ࡞ࡗ
ࡓྠࡌࢧࣥࢦヨᩱ࡟ࡘ࠸࡚ࠊ࡛ࡁࡿࡔࡅከࡃࡢ

(4) Hossain, M. S., Ohde, S., Tanaka. K.,
Sirirattanachai, S., Snidvongs, A. (2008) Oxygenisotope composition in Porites coral from the Northern
Gulf of Thailand: an implication for its skeletal growth.
Bull. Soc. Sea Water Sci., Jpn., 62, 112-113(5) Bogan, R. A. J., Ohde, S., Arakaki, T., Mori, I.,
McLeod, C. W. (2009) Changes in Rainwater pH
associated with increasing atmospheric carbon dioxide
after the industrial revolution. Water Air Soil Pollut.,
196, 263-271ඖ⣲ࡢᐃ㔞ࢆ⾜࠺ணᐃ࡛࠶ࡿࠋࡑࡋ࡚ࠊࢹ࣮ࢱ
⾲ Ⅳ㓟ሷᶆ‽ࡢࣇࢵ⣲ࡢศᯒ⤖ᯝ㸦SSP㸧㸦ᣓᘼࡢᩘ್ࡣศᯒᅇᩘ㸧
&RGH
1R ,1$$
0DWHULDO -&S
±  
FRUDO -'R
±  
GRORPLWH ,&

6SHFWURSKRWRPHWU\/LWHUDWXUHYDOXH

±  ±  ±  ±  ±  

3-14- 373 -

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JAEA-Review 2013-039

⾲  ࢧࣥࢦヨᩱࡢࣇࢵ⣲ศᯒ⤖ᯝ㸦SSP㸧

Sample*1
Location
Genus
88031201
Pohnpei
Porites
88031202
Pohnpei
Porites
880313
Pohnpei
Porites
981101
Khang Khao
Porites
981102
Khang Khao
Porites
981103
Khang Khao
Porites
01031501
Khang Khao
Porites
01031502
Khang Khao
Porites
01031503
Khang Khao
Porites
03040406
Cebu
Porites
030405031
Cebu
Pocillopora
03040403
Cebu
Pocillopora
03040404
Cebu
Porites
03040405
Cebu
Porites
03040406
Cebu
Porites
03040407
Cebu
Porites
03040409
Cebu
Porites
03040410
Cebu
Foliose
03040501
Cebu
Porites
00070401
Mizugama
Porites
00070402
Mizugama
Porites
00070502
Mizugama
Porites
00071601
Mizugama
Porites
00071901
Mizugama
Porites
00071902
Mizugama
Porites
00071903
Mizugama
Porites
00071904
Mizugama
Porites
00081103
Mizugama
Porites
00081208
Mizugama
Porites
00081209
Mizugama
Porites
03073101
Rukan-sho
Porites
03073102
Rukan-sho
Porites
03073104
Rukan-shoPocillopora
03073105
Rukan-sho
Porites
03073106
Rukan-shoPocillopora
03073103
Rukan-sho
Acropora
83021621
Sakai port
Fungia83021622
Sakai port
Porites
83021623
Sakai port
Acropora
83021624
Sakai port
Acropora
83021625
Sakai port
Acropora
83021627
Sakai port
Acropora*1: Sample code gives information on sampling data,
e.g. 88031201 was collected on 12 March 1988

- 374 -

F (ppm)
758
688
693
526
832
620
667
720
698
719
790
743
677
756
552
668
864
636
843
814
840
796
724
780
797
749
824
651
725
850
839
917
896
896
737
826
801
815
1060
1070
1010
974

3-14

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JAEA-Review 2013-039

⾲ 3. ࢧࣥࢦ㦵᱁୰ࡢࣇࢵ⣲ྵ㔞ࡢᖹᆒ್࡜ CaF2ࠊ࠾ࡼࡧᾏỈࡢ ᗘ࡜ CO32-㸦ィ⟬್㸧 

Location㻌

Number 㻌F㻌

CaF2 㻌

Sea surface 㻌CO32- 㻌㻌㻌of samples㻌(ppm)㻌

(μmol/g)㻌

temprature ( )㻌(ȝmol/kg䠅㻌

Pohnpei㻌3㻌

713±32㻌

37.5㻌

28.7(27.5-29.8)㻌

248㻌

Khang Khao㻌6㻌

677±93㻌

35.6㻌

28.4(26.3-30.1)㻌

246㻌

Cebu㻌

10㻌

725±91㻌

38.2㻌

28.3(25.3-30.5)㻌

246㻌

Mizugama㻌

11㻌

777±57㻌

40.9㻌

23.1(19.5-28.9)㻌

216㻌

Rukan-sho㻌6㻌

852±61㻌

44.8㻌

22.7(20.6-30.1)㻌

213㻌

Sakai㻌

6㻌

955±108㻌

50.3㻌

19.6(10.5-27.6)㻌

194㻌

㻝㻜㻜㻜

㻼㼛㼔㼚㼜㼑㼕
㻯㼑㼎㼡㻾㼡㼗㼍㼚㻙㼟㼔㼛㻷㼔㼍㼚㼓㻌㻷㼔㼍㼛㻹㼕㼦㼡㼓㼍㼙㼍
㻿㼍㼗㼍㼕

㻥㻜㻜
㻤㻜㻜
㻣㻜㻜
㻢㻜㻜
㻝㻤㻜

㻞㻜㻜

㻞㻞㻜
㻞㻠㻜
㻯㻻㻟 㻌㻔䃛㼙㼛㼘㻛㼗㼓㻕

㻞㻢㻜

㻞㻙



ᅗ  ࢧࣥࢦ㦵᱁୰ࡢࣇࢵ⣲ྵ㔞㸦ᖹᆒ್㸧࡜ᾏỈࡢ CO32-⃰ᗘ㸦ィ⟬್㸧ࡢ㛵ಀ㸦R2 = 0.922㸧

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JAEA-Review 2013-039

3-15㞤㞝ࢭࣞࣥḞஈ࡟࠾ࡅࡿ㓟໬ࢫࢺࣞࢫ࡜⏕యෆᚤ㔞ඖ⣲ືែ
Dynamics of biotrace elements in selenium deficient female and male rats㐲⸨࿴㇏㸯ࠊᮏ⏣ᬛ㤶Ꮚ㸯ࠊᯇᒸᆂ௓㸯ࠊሯ⏣ṇ㐨㸰㸯᫛࿴⸆⛉኱Ꮫ⸆Ꮫ㒊ࠊ㸰᫂἞኱Ꮫ㎰Ꮫ㒊
Kazutoyo Endo㸯, Chikako Honda㸯, Keisuke Matsuoka㸯, and Masamichi-Tsukada㸰,
1 Showa Pharmacuetical University, Higashi-Tamagawagakuen, Machida, Tokyo, 194-8543,
2 School of Agriculture, Meiji University, Higashi-Mita, Tama-ku, Kawasaki 214-8581⏕యࡢ୺せᡂศඖ⣲ࡣ㓟⣲(O)ࠊⅣ⣲(C)ࠊỈ⣲(H)ࠊ

ࡀ▱ࡽࢀ࡚࠸ࡿࠋࡇࡢࡼ࠺࡟⏕యᚤ㔞㔠ᒓඖ⣲ࡣ㐣❅⣲(N)ࠊ࢝ࣝࢩ࣒࢘(Ca)ࠊࣜࣥ(P)ࠊ◲㯤(S)ࠊ࢝ࣜ

๫ᦤྲྀ࠶ࡿ࠸ࡣḞஈ࡟ࡼࡾᵝࠎ࡞⑌ᝈࡢཎᅉ࡜࡞ࡿ

࣒࢘(K)ࠊࢼࢺ࣒ࣜ࢘(Na)ࠊሷ⣲(Cl)ࠊཬࡧ࣐ࢢࢿࢩ

ࡇ࡜ࡀ᫂ࡽ࠿࡟ࡉࢀ࡚࠸ࡿࠋ ⏕య࡟Ꮡᅾࡍࡿᚲ㡲ᚤ࣒࢘(Mg)࡛࠶ࡾࠊࡑࢀࡽࢆྜࢃࡏࡿ࡜ࠊయෆ࡟Ꮡᅾ

㔞㔠ᒓඖ⣲ࡣࡑࡢඖ⣲ࡀ༢⊂࡛⏕యᶵ⬟࡟㛵୚ࡋ࡚ࡍࡿ඲ඖ⣲ࡢ 99㸣௨ୖ࡟࡞ࡿࠋ ୍᪉ࠊ⏕యᚤ㔞ඖ࠸ࡿࡔࡅ࡛࡞ࡃࠊ௚ࡢඖ⣲࡜஫࠸࡟స⏝ࡋࠊࡑࡢඖ

⣲ࡢయෆᏑᅾ㔞ࡣ඲ඖ⣲㔞ࡢ 1㸣ᮍ‶࡛࠶ࡾࠊࡑࢀ

⣲㛫┦஫స⏝ࡀ⏕⌮άᛶ࡟ᙳ㡪ࢆཬࡰࡋ࡚࠸ࡿࠋ≉ࡽࡢṤ࡝ࡀ⺮ⓑ㉁ࡸ㓝⣲࡜⤖ྜࡋ࡚Ꮡᅾࡋ࡚࠸ࡿࠋ

࡟ Se, Fe, Zn, Cu, Mn, Co ࡣ㓝⣲ࡸࣅࢱ࣑ࣥࡢάᛶ

⏕య࡟Ꮡᅾࡍࡿ㔠ᒓඖ⣲ࡢ࠺ࡕࠊࣄࢺࡢᚲ㡲ᚤ㔞ඖ୰ᚰ࡜ࡋ࡚Ꮡᅾࡋࠊ⏕యෆ࡛ࡢ㓟໬㑏ඖ཯ᛂࡢㄪ⠇⣲࡜ࡋ࡚᫂ࡽ࠿࡟ࡉࢀ࡚࠸ࡿࡶࡢࡣࢭࣞࣥ(Se), 㕲࡟῝ࡃ㛵ࢃࡗ࡚࠸ࡿࠋSe ࡣࠊ⏕యෆ࡛ࡣࢢࣝࢱࢳ࢜

(Fe), ள㖄(Zn), 㖡(Cu), ࣐ࣥ࢞ࣥ(Mn), ࣚ࢘⣲(I),

ࣥ࣌ࣝ࢜࢟ࢩࢲ࣮ࢮ(GPX-Px)ࡢάᛶ୰ᚰ࡛ࠊ㐣㓟໬ࣔࣜࣈࢸࣥ(Mo), ࢡ࣒ࣟ(Cr), ཬࡧࢥࣂࣝࢺ(Co)ࡢ

Ỉ⣲(H2O2)ࡢᾘཤ࡟㛵ಀࡋ࡚࠸ࡿࠋGPX-Px ࠾ࡶ࡟

9 ඖ⣲࡛࠶ࡿࠋ⏕యࢆྲྀࡾᕳࡃ⎔ቃ࡟ࡣከࡃࡢ㔠ᒓ⫢⮚࡟ከࡃᏑᅾࡋ࡚࠾ࡾࠊࡇࡢ㓝⣲ࡢάᛶࡀపୗࡋ

ඖ⣲ࡀᏑᅾࡋࠊ⏕య࡟࡜ࡗ࡚ᚲ㡲࡞㔠ᒓඖ⣲ࡔࡅ࡛ࡓ≧ែ࡛ࡣࠊ⫢⮚ࡣ H2O2 ࢆ௓ࡋࡓ㓟໬ⓗࢫࢺࣞࢫ࡞ࡃࠊ᭷ᐖ࡞ඖ⣲ࡶඹ࡟ࠊ⏕యෆ࡬ྲྀࡾ㎸ࡲࢀࡿྍ࡟᭚ࡉࢀࡿ࡜⪃࠼ࡽࢀࡿࠋࡇࢀࡲ࡛ࡢ◊✲࡛ࡣࠊ8⬟ᛶࡀᴟࡵ࡚㧗࠸ࠋࡲࡓࠊࡓ࡜࠼ࠊᚲ㡲ඖ⣲࡛࠶ࡗ㐌㱋㞝ᛶ Se-Ḟஈࣛࢵࢺࡢ⫢⮚ࠊ࠾ࡼࡧࡑࡢ௚ࡢ⮚࡚ࡶࠊࡑࢀࡽࡢඖ⣲ࢆ㐣๫࡟ᦤྲྀࡋࡓሙྜࠊ⏕య࡟ჾࡢඖ⣲㔞ࢆ ᐃࡋࡓࠋᑐࡋ࡚ᝏᙳ㡪ࢆ୚࠼ࡿࡇ࡜ࡀ࠶ࡿࠋ୍᪉ࠊᚲ㡲ඖ⣲ᮏ◊✲࡛ࡣࠊ㸯㸧㓟໬ࢫࢺࣞࢫࡢࣔࢹࣝ࡜ࡋ࡚㞤ᛶࡀḞஈࡍࡿ࡜⏕య࡟ᵝࠎ࡞㞀ᐖࢆᘬࡁ㉳ࡇࡍࡇ࡜࠾ࡼࡧ㞝ᛶ Se Ḟஈࣛࢵࢺࢆࣔࢹࣝ࡟⏝࠸࡚ࠊୖグ◊✲᪋タ࡜᪋タྡ㸸-55 ' ࣃ࢖ࣉ             ◊✲ศ㔝㸸ᨺᑕ໬ศᯒࠊᚤ㔞ศᯒ - 376 -

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JAEA-Review 2013-039

Fig. 1 ⫢⮚ࠊ⭈⮚ࠊ⭁⮚ࠊ⬻࡟࠾ࡅࡿ Se 㔞ࡢẚ㍑㸹 ᕥ) 㞝ᛶࣛࢵࢺࠊྑ 㞤ᛶࣛࢵࢺ

Fig. 2 ⫢⮚ࠊ⭈⮚ࠊ⭁⮚ࠊ⬻࡟࠾ࡅࡿ Fe 㔞ࡢẚ㍑㸹 ᕥ) 㞝ᛶࣛࢵࢺࠊྑ 㞤ᛶࣛࢵࢺᚤ㔞ඖ⣲ࡢ⮚ჾศᕸ࡜ᢠ㓟໬㓝⣲ࡸᢠ㓟໬≀㉁࡟࠾

(SeC)⩌ࠊ࠾ࡼࡧ Se Ḟஈ(SeD)⩌ࡢ⫢⮚ࠊ⭈⮚ࠊ⭁ࡅࡿ㞤㞝ࡢᕪ␗ࢆẚ㍑᳨ウࡍࡿࡇ࡜ࠊ㸰㸧㞝ᛶ 6H⮚ࠊ࠾ࡼࡧ⬻୰ࡢ Se 㔞ࢆ Fig.1 ࡟♧ࡋࡓࠋSe ࡟㛵Ḟஈࣛࢵࢺࢆ⏝࠸࡚ࠊ㛗ᮇ㛫ࡢ 6H Ḟஈࡀཬࡰࡍ⏕యࡋ࡚㞤㞝ࢆẚ㍑ࡍࡿ࡜ࠊSe 㔞ࡢ༑ศ࡞ SeC ⩌࡛ࡣᚤ㔞ඖ⣲ࡢ⮚ჾศᕸࡢኚ໬ࢆ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࢆ┠ྛ⮚ჾ࡜ࡶ㞤ᛶࣛࢵࢺࡢ࡯࠺ࡀࠊྛ⮚ჾ࡬ࡢྲྀ㎸ࡳⓗ࡟ࡋࡓࠋ⏕యෆ࡛ࡢάᛶ㓟⣲ࡢ⏕ᡂ࡜ᾘཤ࡟㛵ࢃࡀከࡃ࡞ࡗ࡚࠸ࡿࠋࡇࢀࡣࠊู࡟ ᐃࡋࡓ GSH-Pxࡿᢠ㓟໬㓝⣲࣭࠶ࡿ࠸ࡣᢠ㓟໬≀㉁࡛࠶ࡿ *3; άᛶࠊάᛶࡀ㞤ᛶ࡟࠾࠸࡚᭷ព࡟㧗࠸ࡇ࡜࡟ᑐᛂࡋ࡚࠸ࡿࠋ

GSH 㔞ࠊSOD άᛶࠊ⏕యࡢ㓟໬ࢫࢺࣞࢫ࣐࣮࣮࢝

normal ⩌ࠊSeC ⩌ࠊ࠾ࡼࡧ SeD ⩌ࡢ⫢⮚ࠊ⭈⮚ࠊ࡛࠶ࡿ TBARS ್ࠊ⏕యᚤ㔞ඖ⣲࡛࠶ࡿ Se, Fe, Co,⭁⮚ࠊ࠾ࡼࡧ⬻୰ࡢ Fe 㔞ࢆ Fig.2 ࡟♧ࡋࡓࠋ㞤ᛶ࡜

Cu, Zn ࢆᨺᑕ໬ศᯒ࡟ࡼࡗ࡚

ẚ㍑ࡋ࡚㞤ᛶࡣࠊ࡝ࡢ⮚ჾࡶ Fe 㔞ࡀ 1.5㹼2 ಸ⛬ᗘᐃࡋࠊࡑࢀࡒࢀࡢ㔞ࢆẚ㍑ࡋࡓࠋ

ከ࠸ࠋFe ㈓ⶶ࡜௦ㅰ࡟୺せ࡞ᙺ๭ࢆࡍࡿ⭁⮚࡟࠾࠸㸯㸧㞤㞝ࣛࢵࢺࡢ Se ࠾ࡼࡧ Fe 㔞ࡢྲྀ㎸ࡳ㔞࡚㞤㞝࡛ࡣ␗࡞ࡗ࡚࠸ࡓࠋ8 㐌㱋ࡢ㞤㞝ࣛࢵࢺ⫢⮚8 㐌㱋ࡢ㞤㞝ࡢṇᖖ(normal)⩌ࠊSe ࢥࣥࢺ࣮ࣟࣝ

୰ࡢ SOD άᛶࢆᐃࡋࡓ⤖ᯝࠊSeC ⩌࡜ SeD ⩌ࢆ

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JAEA-Review 2013-039ẚ㍑ࡍࡿ࡜㞝ᛶ࡟࠾࠸࡚ࡣ୧⩌࡜ࡶ᭷ព࡞ᕪࡣ࡞࠿

㔞ඖ⣲࡜ࡢ㛵ಀࡀࡼࡾ᫂░࡟࡞ࡿ࡜ᛮࢃࢀࡿࠋࡲࡓࠊ

ࡗࡓࠋ୍᪉ࠊ㞤ᛶ࡛ࡣ SeC ⩌ࡢ࡯࠺ࡀ㧗࠸್ࡀᚓࡽ

㛗ᮇ㛫ࡢ Se-Ḟஈࡢᙳ㡪࡟ࡘ࠸࡚ࡣࠊࡇࢀࡲ࡛ㄪ࡭

ࢀࡓࠋࡇࢀࡣࠊ㞤ᛶࡢ࡯࠺ࡀ GSH-Px άᛶࡀ㧗ࡃࠊࡽࢀ࡚࠸࡞࠸ࠋᮏ◊✲࡛ࡣ 50 㐌㱋ࡢᮇ㛫࡟ரࡿ Se㐣㓟໬Ỉ⣲ࢆ㑏ඖࡍࡿࡍࡿ⬟ຊࡀ㧗ࡃࡇ࡜࡜ࠊࡑࢀ

Ḟஈࣛࢵࢺ⫢⮚୰ࡢ⏕యෆ㓟໬㑏ඖ࡟㛵ಀࡢ࠶ࡿᚤ

࡟క࠸ࢫ࣮ࣃ࣮࢜࢟ࢧ࢖ࢻ㸦࣭O2-㸧࠿ࡽ㐣㓟໬Ỉ⣲㔞ඖ⣲㸦Mn, Fe, Co, Zn, Cu, Se㸧ྵ㔞ࡢኚ໬ࢆほᐹࢆ⏕ᡂࡍࡿ SOD άᛶࡀ㧗ࡃ࡞ࡗ࡚࠸ࡿ࡜ࡶ⪃࠼ࡽࡋࡓࠋ
Fig. 3 ࡟ࡣࠊ⮚ჾ୰ࡢ Se 㔞ࡢ㐌㱋౫Ꮡᛶࢆ♧ࡋࡓࠋࢀࡿࠋࡇࢀࡲ࡛ࠊ㞝ᛶ࡟ࡘ࠸࡚ᐇ㦂ࢆ⥆ࡅ࡚ࡁ࡚௒
ᅇ㞤ᛶ࡟ࡘ࠸࡚ᐇ㦂ࢆ⾜࠸ࠊᇶ♏ࢹ࣮ࢱࢆᚓࡿࡇ࡜

SeD ⩌࡛ࡣ 4 㐌㱋࡛ᐃࡉࢀࡓ㸦0.27s0.19 mg/kg,

ࡀ࡛ࡁࡓࠋ㞤ᛶ࡟㛵ࡋ࡚ࡣࡉࡽ࡟ࢹ࣮ࢱࡢ⵳✚࡜ẚ

n=3㸧ࡢᑡ㔞ࢆ㝖࠸࡚ࡣࠊ࡯࡜ࢇ࡝᳨ฟ㝈⏺࡟㏆࠸

㍑ࡀᚲせ࡛࠶ࡿࠋ

್ࢆ♧ࡋࡓࠋࡋ࠿ࡋࠊSe ࡣࡍ࡭࡚ࡢ SeD ⩌ࡢ⭈⮚㸰㸧㛗ᮇ㛫ࡢ Se-Ḟஈࡢᙳ㡪࡛ࡇࢀࡲ࡛࡟ Se Ḟஈࣛࢵࢺࡢ㣫⫱㛤ጞ㐌㱋ཬࡧࡑ࡟࠾࠸࡚ࡣࡈࡃప࠸࡛ࣞ࣋ࣝ

ᐃࡉࢀࡓࠋ⭁⮚࡛ࡣࠊSe ࡣ 4-,12-,16-, 20 㐌㱋ᐃࡉࢀࡓࡀࠊ8-, 50-ࡢ㣫⫱ᮇ㛫࡟క࠸㐣㓟໬Ỉ⣲ࣞ࣋ࣝ࡞࡝ࡢ㓟໬ࢫࢺ㐌㱋࡛ࡣ᳨ฟࡉࢀ࡞࠿ࡗࡓࠋṇᖖ⩌ࡢ⮚ჾࡢ୰࡛ Seࣞࢫ࡟ኚ໬ࡀ⏕ࡌࡿࡇ࡜ࢆ᫂ࡽ࠿࡟ࡋ࡚ࡁࡓࠋࡲࡓࠊ

㔞ࡣࠊྠࡌ㐌㱋ࡢ SeD ⩌ࡼࡾࡶ࠿࡞ࡾ㧗࠸ࠋṇᖖ⩌Se Ḟஈࣛࢵࢺཬࡧࣅࢱ࣑ࣥ E Ḟஈࣛࢵࢺ࡛ࡣඹ࡟

ࣛࢵࢺࡢ Se 㔞ࡣࠊࡑࡢ㏿ᗘࡣ␗࡞ࡿࡶࡢࡢࠊ ᐃ⫢⮚࡛ࡢ Fe ࡢ⵳✚ࡀほᐹࡉࢀ࡚࠾ࡾࠊSe Ḟஈື≀ࡋࡓࡍ࡭࡚ࡢ⮚ჾ࡛ቑຍࡍࡿഴྥ࡟࠶ࡗࡓࠋ㝿❧ࡗ࡛ࡣ㐌㱋࡟క࠺ Fe ࡢືែኚ໬ࡶண᝿ࡉࢀ࡚࠸ࡿࠋ

࡚㧗࠸್ࡢ Se ࡀࠊ50 㐌㱋ṇᖖ⩌ࣛࢵࢺࡢ⭈⮚࡛Se Ḟஈࡢᮇ㛫ࢆᘏ㛗ࡉࡏࢀࡤࠊ⏕య࡟୚࠼ࡽࢀࡿ㓟ᐃࡉࢀࡓࠋ Se 㔞࡟ᐦ᥋࡟㛵㐃ࡋ࡚࠸ࡿ⫢⮚ࡢ໬ࢫࢺࣞࢫ࡟ኚ໬ࢆ⏕ࡌࠊࡑࢀ࡟క࠸ᚤ㔞ඖ⣲ືែ

GSH-Px ࡢ㐌㱋౫Ꮡ㸦Fig.3A㸧࡜ṇᖖ⩌ࣛࢵࢺࡢࡢኚ໬ࡶண᝿ࡉࢀࠊ㓟໬ࢫࢺࣞࢫࡢኚ໬࡜ࡑࢀ࡟క

GSH-Px ࡣ┦㛵ࡋ࡚࠸ࡿࠋ

࠺ᚤ㔞ඖ⣲ືែࢆᢕᥱࡍࡿࡇ࡜࡛㓟໬ࢫࢺࣞࢫ࡜ᚤ

3-15



- 378 -

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800

1600

12

600

Liver

8
4
0

200
(2)

0

10

Selenium (mg/kg)
Selenium (mg/kg)

50

60

**
**

1200

**

12
**

8

**

*’

*’

**

4
0

20

**

10

20
30
40
Age (week)

50

1

400

0
10

8
4

(1)

0

(1)

(2)

*

*

(2) (2)

(2)

*’

10

20
30
40
Age (week)

50

60

800
400

*

*’

0

C

60

50

**

1200

*

*’

10

*’

20
30
40
Age (week)

50

60

20
30
40
Age (week)

50

60

Spleen

20000
15000
10000

*
**

5000

*

(1)

0

20
30
40
Age (week)

Kidney

1600

25000

12

2

800

0

Spleen

16

**

*’

0

B

60

3

**

0

A

Kidney

16

0

B

20
30
40
Age (week)

0

4

Liver

2000

20

C

400

**

NormalSeD
P-450 (nmol/g prot.)

16

Iron (mg/kg)

1000

2000

20

Iron (mg/kg)

A

Normal GSH-Px
SeD GSH-Px

Iron (mg/kg)

Selenium (mg/kg)

NormalSeD

GSH-Px activity (U/mg prot.)

JAEA-Review 2013-039

0
0

10

Fig. 4 ⫢⮚ࠊ⭈⮚ࠊ⭁⮚୰ࡢ )H 㔞

Fig.3 ⫢⮚ࠊ⭈⮚ࠊ⭁⮚୰ࡢ Se 㔞

Fig.4 ࡟ࡣ࠸ࡃࡘ࠿ࡢ⮚ჾ୰ࡢ Fe 㔞ࢆ♧ࡋࡓࠋṇ⭁⮚୰ࡢ Fe 㔞ࡣࠊ௚ࡢ⮚ჾࡼࡾࡶ 1㹼2 ᱆㧗࠸್ᖖ⩌ࣛࢵࢺ⫢⮚୰ࡢ㕲㔞ࡣࠊ4 㐌㱋࡛ 800mg/kg ࠿ࢆ♧ࡋࡓࠋSeD ⩌࡜ṇᖖ⩌ࡢ୧᪉ࡢࣛࢵࢺࡢ⭁⮚୰

ࡽ 20 㐌㱋࡟࠿ࡅ࡚ࡣᚎࠎ࡟ῶᑡࡋࠊ50 㐌㱋࡛ࡣ⫢ࡢ Fe 㔞ࡣࠊ8 㐌㱋ࡲ࡛ࡣࠊẚ㍑ⓗᑡ࡞ࡃࠊ8 㐌㱋⮚࡛ࡣ 1300mg/kg ࢆࡋࡵࡋࡓࠋ20 㐌㱋ࡼࡾࡶⱝ࠸

௨㝆࡟ቑຍࡋጞࡵࡓࠋṇᖖࣛࢵࢺ⩌ࡢ⭁⮚୰ࡢ Fe⩌࡛ࡣ SeD ࣛࢵࢺ⩌ࡢ Fe 㔞ࡣṇᖖ⩌ࡼࡾࡶከ࠸ࡀࠊ

ࡣ 50 㐌㱋࡟⮳ࡿࡲ࡛ቑຍࡋࡓࠋ20 㐌㱋௨㝆ῶᑡࡋ40 㐌㱋ࡢ SeD ࣛࢵࢺ⩌࡛ࡣྠࡌ㐌㱋ࡢṇᖖ⩌ࡼࡾࡓࠋ50 㐌㱋ࡢ SeD ⩌ࡣࠊṇᖖ⩌ࡼࡾࡶ㝿❧ࡗ࡚ᑡࡶ Fe ࣞ࣋ࣝࡣప࠿ࡗࡓࠋSeD ⩌ࡢࣛࢵࢺ⫢⮚ࡢ࡞࠸㔞ࢆ♧ࡋࡓࠋSeD ࣛࢵࢺࡢࢩࢺࢡ࣒ࣟ P-450

Fe 㔞ࡣ㐌㱋࡟౫Ꮡࡋ࡚ 780-1500mg/kg ࡛࠶ࡾࠊࡑ

άᛶ㸦Fig.㸲A㸧ࡣ SeD ࣛࢵࢺ⭁⮚ࡢ )H 㔞࡟ྠᮇࡢᖹᆒ࡟౫Ꮡࡋ࡚࠸ࡓࠋSeD ࣛࢵࢺ⭈⮚୰ࡢ Fe 㔞ࡋ࡚࠸ࡿࡼ࠺࡟ぢ࠼ࡿࠋࡋ࠿ࡋࠊṇᖖ⩌ࣛࢵࢺ⫢⮚ࡣ 190㸫370mg/kg ࡛࠶ࡾࠊ࠶ࡲࡾኚືࡣ↓࠸ࠋ୍ࡢࢩࢺࢡ࣒ࣟ P-450 άᛶࡣ Fe 㔞࡜ࡣ㛵㐃ࡋ࡚࠸࡞᪉ࠊṇᖖ⩌ࣛࢵࢺ⭈⮚୰ Fe 㔞ࡣ 4 㐌㱋࡛ 260mg/kgࠊ࠸ࡼ࠺࡛࠶ࡿࠋ

3-15

50 㐌㱋࡛ࡣ 1160mg/kg ࡛࠶ࡗࡓࠋ      - 379 -

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JAEA-Review 2013-039

Zn ࡣࠊFe ࡜␗࡞ࡾ㐌㱋࡟ᑐࡋ࡚⫢⮚ࠊ⭈⮚ࠊ⭁⮚

2㸧Oxidative stress of selenium deficiency and mineralbalance in rats, Y. Sakuma, K. Matsuoka, C. Honda,࡟࠾࠸࡚ 50 㐌㱋࡟⮳ࡿࡲ࡛ࠊኚ໬ࡀᑡ࡞࠿ࡗࡓࠋ

K. Matsumoto, K. Endo, Int. Symp. Metallomics,ࡲࡓࠊṇᖖ⩌࡜ SeD ⩌࡜ࡢ㛫࡟ࡣⴭࡋ࠸ᕪࡣ࡞࠿ࡗ

Nov.28 –Dec.1, Nagoya (2007).

ࡓࠋࡉࡽ࡟⮚ჾ୰ࡢ Zn 㔞ࡣࠊ⏕ᾭࢆ㏻ࡋ࡚ኚືࡣ

ᅜ㝿఍㆟ Proceeding㸸ᑡ࡞࠿ࡗࡓࠋ࡞࠿࡛ࡶ⭁⮚୰ࡢ Zn 㔞ࡣࡶࡗ࡜ࡶᕪ㸯)Y. Sakuma, K. Matsuoka, C. Honda, K. Matsumoto,
K. Endo: Dynamics of redox related elements (Fe,ࡀᑡ࡞࠿ࡗࡓࠋ

Co, Zn, and Se) and oxidative stress caused bySe-deficiency in rats. J. Radioanal. Nucl. Chem.
278(2008)591-594.

࠙ㅰ㎡ࠚ ᮏ◊✲ࢆ㐍ࡵࡿ࡟࠶ࡓࡾࠊ୰ᛶᏊ↷ᑕ࡟ࡈ༠ຊࢆ㡬࠸ࡓᮾி኱Ꮫ኱Ꮫ㝔ᕤᏛ◊✲⛉ᑓ㛛⫋኱ㄽᩥ㸸
1㸧Y. Sakuma, J. Sasaki, A. Futami, K. Yamasaki, K.

Ꮫ㝔ࡢ⃝⏿ᾈஅẶࠊᕝᡭ ⛱Ặࠊ▼ᮏ ග᠇Ặ࡟῝

Matsuoka, C. Honda, K. Endo, M. Tsukada,ࡃឤㅰ࠸ࡓࡋࡲࡍࠋᮏ◊✲࡛ࡣ⛉Ꮫ◊✲㈝⿵ຓ㔠ᇶ

Changes in the components of biliary and plasma
lipids in selenium-deficient rats, Chem. Phys.

┙◊✲ &  ࡢ୍㒊ࢆ౑⏝ࡋࡓࠋ

Lipids 148 (2007) 70-76.

2) K Matsumoto, S.Terada, M. Ariyosh, A. Okajo, A.

࠙ᡂᯝࡢබ⾲ࠚ

Hisamatsu, I. Ui, K. Endo, The effect ofᏛ఍Ⓨ⾲➼㸸
1) ࢭࣞࣥḞஈ࡟ࡼࡿ㓟໬ࢫࢺࣞࢫ࡜⏕యෆᚤ㔞ඖ⣲ືែ࡟㛵ࡍࡿ◊✲ (᫛࿴⸆኱) ࠐ㐲⸨࿴㇏ࠊబஂ㛫Ὀரࠊ㟢ᮌ⪽ྐࠊ㛗ᒣᩔᏊࠊᯇᒸᆂ௓ࠊ
ᮏ⏣ᬛ㤶Ꮚ㸦ᨺ་◊㸧ᯇᮏㅬ୍㑻 ➨ 127 ᅇ᪥ᮏlong-running severe selenium-deficiency on theamount of iron and zinc in the organ of rats,
Molecules 14 (2009) 4440-4453.

3-15⸆Ꮫ఍ᖺ఍ 㸦ᐩᒣ኱ 2007 ᖺ 3 ᭶ 28㸫30 ᪥㸧ࠋ- 380 -

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JAEA-Review 2013-039

3-16୰ᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡿ⏕≀ヨᩱ୰ࡢ࢔࣑ࣝࢽ࣒࢘ศᯒ
Aluminum Analysis in Biological Materials by Instrumental Neutron Activation Analysis
ຍ⸨ὒ㸦㤳㒔኱Ꮫᮾி㸧
Y. Katoh (Tokyo Metropolitan University)ᒣᮏዲ⏨㸦୕㔜኱Ꮫ♫఍㐃ᦠ◊✲ࢭࣥࢱ࣮㸧
Y. Yamamoto (Mie University Social Cooperation Research Center)

INTRODUCTION
The Al determination of various materials by
this method has been employed. However, theapplication of INAA for biological materials has
the following problems: 1) competing interference
reactions from the elements Si and P, and 2)
interference created by irradiation from
impurities in wrapping material of the specimenmaterial. INAA has contributed little to Al value
certification for biological standard materials, etc,
because the above factors prevent INAA fromdetermining accurate Al concentrations. In thisstudy, the concentrations of Si and P were
determined by an alternative nuclear method,
Particle Induced X-ray Emission (PIXE) for Si
and P, and the ǃ-ray measurement with Liquid
Scintillation Counting (LSC) of 32P produced by
31P(n,Ǆ)32P
in the specimens used for Al
determination.
EXPERIMENTS AND MATERIALSThe Certified Reference Material (CRM) andStandard Reference Material (SRM) of the 6
botanical and 12 animal specimens used for Al
determination are shown in Table 1. The samples
that were irradiated were about 50 mg of CRM,
SRM. The comparative standard for Al was
prepared through deposition of an atomic
absorption solution (Wako Pure Chemicals Co.
Ltd.). The capsules were irradiated in thepneumatic tube of the JRR-4 reactor. The
irradiation time was 40 seconds, and theirradiated samples with exchanged outer bags
were immediately measured for 1779 keV Ǆ-ray of
28Al using a high pure Ge semiconductor detector

Table 1

List of CRMs and SRMs
Abbreviation

Material

Supplier

Algae

IAEA

Algae-391

Algae

IAEA

Algae-392(in this report)

Algae

IAEA

Algae-393

Animal Bone

IAEA

AB

Animal Muscle

IAEA

AM

Bovine Liver

NBS

BL

Bovine Liver

NIST

BLa

Kale

BOWEN

BK

Dogfish Mussel

NRCC

DORM-2Horse Kidney

IAEA

HK

NRCC

TORT-1NRCC

TORT-2

Milk Powder

IAEA

MP

Mussel Tissue

BCR

MT

Orchard Leaves

NBS

OL

Pig Kidney

BCR

PK

Pine Needle

NIST

PNa

Whey Powder

IAEA

WP

Lobster
Hepatopancreas
Lobster
Hepatopancreas

IAEA : International Atomic Energy Agency24
NBS: National Bureau of Standard
NIST: National Institute of Standards and Technology
NRCC: National Research Council Canada
BCR: Community Bureau of Reference

coupled to a multi-channel pulse-height analyzer
for 100 seconds.
For the determination of the interference
factors from Si and P, SiO2 and (NH4)2HPO4 werealso
irradiatedrespectively.
Forthe

JRR-4㸪 PN Ẽ㏦⟶↷ᑕタഛ㸪⏕≀ヨᩱᨺᑕ໬ศᯒ

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JAEA-Review 2013-039

determination of P in specimens using the LSC
method, the irradiated specimens after the Ǆ-ray
measurement were subjected to dissolution by the
microwave-assisted high pressure digestion withthe apparatus developed by Fuse Lim. Co.. These
specimens and the (NH4)2HPO4 powder weredissolved with 1 ml of concentrated HNO3
(ultrapure general reagent; Wako Pure Chemical
Inc. Ltd.). The activities of a 200 Ǎl solution
containing 32P with a half-life (14.26 d) and a
ǃ-ray maximum energy (1.711 MeV) were
measured following the decay. The counting of
ǃ-rays was conducted with the Packard Co. Ltd.
LSC 2900TR using a cocktail (Soluscint XR,
National Diagnostics, Inc.). The determination of
32P activities were interfered by the ǃ-rays fromnuclides, 33P, 35S and 45Ca due to S, Cl and Ca,
respectively. The high purity of compounds
containing S, Cl and Ca were used to obtain thequantitative interference factors from eachelement.
The specimen solutions dissolved by theabove-mentioned method were also applied to the
PIXE method by adding the atomic absorption
solution of In (Wako Pure Chemical Inc. Ltd 1000ppm.) as an internal standard. Five Ǎl of thesolution was dropped on a 4 Ǎm thick backing film
(polypropylene, Toray Ltd.) and dried. The
polyethylene products could not been digested
and directly were irradiated. The target films
were bombarded by a proton beam at the Japan
Radioisotope Association Nishina Memorial
Cyclotron Center in Japan. The energy, flux, anddiameter of the proton beam were 2.9 MeV, 50 nA
and 6 mm, respectively. The induced X-rays were
measured by two Si(Li) semiconductor detectors.
RESULTS AND DISCUSSION
The reliability for theP determination by PIXE,
and the P determination by LSC was confirmed
by comparisons with certified values for various
biological CRMs and SRMs. The results areshown in Table 2. Except for P, the Si levels were
almost below the detection limit.
The
contributions from Si to the Al values in thematerials were neglected in spite of the larger
interfering factor. The P values by both methods
are consistent and either method is applicable for

Table 2Concentrations of phosphorus in biological CRMs
and SRMs

Materials
Algae-391

P (Ǎg/g dry)
PIXE

LSC

Reference

12400

14900

14200**(1)

Algae -392

4500

5830

5490**(1)

Algae-393

17200

18100

15600**

(1)

AB

NC

93900

100200*

(2)

AM

6300

7000

6830*

(3)

BL

13500

11800

10500*

(4)

BLa

12500

11500

11100*

(5)

BK

4200

5490

4880*

(6)

DORM-2

9600

6390

HK

11600

12800

11200*(7)

TORT-1

5700

8880

8790*

(6)

TORT-2

11000

6390

MP

7400

10100

9100**

(6)

MT

5700

6930

6070**

(8)

OL

1500

2300

2100*

(4)

PK

12800

12800

12000**

(9)

PNa

1100

1030

1070*

(10)

WP

16200

16400

16210*(11)* Certified value, ** Information value

determination of P in materials. The value in AB
could not be calculated due to the strong
characteristic X-ray from the concentration of Ca(21.2 % (2)). In the exact determination of P, the
PIXE is generally disadvantaged by spectral
bremsstrahlung in the light elements region.
However, the results can be obtained at a short
experimental time.
In case of the LSC method, the measurement that
follows the decay of the ǃ-ray requires a long time.
The LSC method of counting 32P also has aadditional disadvantage. The ǃ-ray counting of
biological specimens by LSC has interference
from the characteristic elements in biological
specimens. These elements are abundant inbiological materials.
In LSC, activities were counted for the total
ǃ-rays over the 3 keV of energy due to the highdegree of differential quenching with eachspecimen. These ǃ-ray measurements were
followed for six months and the decay curves wereanalyzed. The total ǃ-rays contained, 32P derived
from P, 32P from S, 33P from Cl, 35S from S and Cl,- 382 -

3-16
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JAEA-Review 2013-039

and 45Ca derived from Ca respectively. The decay
curve of WP, for example, is shown in Figure 1. In
this figure, the dotted lines represent thetheoretical decay curves of 32P, 33P and 35S,
respectively. The contribution from 33P and 35S isapparent. The contributions from 35S derived
from S and /or Cl were detected in all specimens,
and the contribution from 33P derived from Cl was
also detected in the case of PK, DORM-2, TORT-2
and WP. The total 32P count is influenced by theconcentration of S and Cl in the specimens. The
large contribution of the 35S activities caused by S
and Cl to the total counts could be avoided bycarefully cutting the low energy ǃ-rays in the LSC
method, since the ǃ-ray energy of 32P and 35S arelargely different. The interference from 47Ca could
be avoided by counting after about two weeks
except for the bone specimen. A careful analysis of
the decay curves is required, in the case of HK(12600 Ǎg/g), TORT-1 (55800), TORT-2 (17500),
MT (27800) and WP (69200), which contain very
Table 3
Materials

C.R. =(non corrected Al value)  (corrected Al value)u 100
corrected Al value

The non corrected values were the mean values of
6 replicate analyses with one standard deviation.
The corrected P values were calculated using themean P values. The corrected values are, inbotanical CRMs and SRMs, lower than thereference values for the Algae series, although theConcentrations of Al in CRMs and SRMs

This study (Ǎg/g dry)
Non-correctedhigh concentrations of Cl, respectively. The
concentration of interfering elements in LSC canbedeterminedbysimultaneous
Ǆ-ray28
spectrometry in measurement of
Al in anobjective specimen. The P values obtained by LSC,
except for AB, were adopted in this study.
The Al concentrations corrected for P for
botanical and animal CRMs and SRMs are shownin Table 3. The Contribution Rate (C.R. (%)),
which refers to the degree of the interference isdefined by following the equation,

C.R.

Corrected(%)

References

Botanical tissues
Algae-391

19.9s1.2

7.5

165

12.5** (1), 4.5*** (12)Algae-392

36.7s1.4

32.2

1437.2** (1), 30.3*** (12)Algae-393

107s3

90

19

98.1** (1), 71.6*** (12)BK

44.0s2.539.8

11

39.9** (6)

OL

429s9

427

0.5

420*** (4)PNa

587s13586

0.2

580* (10)AB

99.1s8.6

5.2

1800

101**(2)AM

12.4s2.0

6.1

103

10**(3)BL

13.4s0.8

NC

16** (13)BLa12.3s1.2NC

2** (13) , 0.6**(15)DORM-221.2s3.6

11.6

HK

11.4s1.3

NC

TORT-139.4s5.7

33.7

17

TORT-2

48.5s7.6

37.5

29

MP

11.7s0.7

4.3

172

Animal tissues

83

10.9*(16)77.7*** (7 )MT

15.2s1.9

8.3

83

PK

19.4s1.8

6.6

194

WP

57.1s2.9

40.7

4043*** (14)53**(11)* Certified value, ** Information value, *** Literature value, NC; Not detected- 383 -

3-16

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JAEA-Review 2013-039

results of BK, OL and PNa are consistent with thecertified or information values. Most of the
botanical materials contained high levels of Al,
and while the concentrations of the interference
elements are lower in comparison with animal
materials, the C.R. ratios varied from 0.2 % toabout 11 %. The correction for P was in somecases necessary, even for the botanical material.
The relatively higher C.R ratios were obtained for
the Algae series and for BK.
Specifically, Algae-1 which has a lower Al
value and a much higher P value, and thisinfluence from P value should be re-examined toconfirm the Al reference value (1). The higher
information values of Al for the Algae series may
be influenced by INAA results. For this series, theresults by Kawamoto et al. (12) by using ICP-MS
were consistent with the corrected values
obtained here. The results in this study also
agreed with the reference value for BK. In
comparing the present results with those ofanimal CRMs and SRMs, agreement is excellent
for DORM-2.The reference value of DORM-2 was
obtained by using the analytical methods except
for those obtained by NAA. For WP, the difference
between the information value and that in thisstudy is significant. In a detailed examination of
the IAEA values (11), the IAEA mean value, 57.8
Ǎg/g compiled by only the INAA method, was very
consistent with the non-corrected value in thisstudy.
The IAEA certified value for this material
may be also influenced by the contribution of the
non-corrected results obtained by INAA in thecertification. This also applies to the case of BL,
BLa and HK. The higher Al value of HK by IAEA
was obtained from little study and the IAEA
value ( Ҹ 10 Ǎg/g) by INAA agreed with the
non-corrected value in this study (7). The Alvalues in BL compiled by INAA varied in rangesof <3-65 Ǎg/g (2), the Al abundance in thismaterial might be naturally inhomogeneous. For
BL, Aluminum could not be detected by correctionin this study (detection limit: 0.06 Ǎg). The C.R.
value for AB, derived from very the high P value
in this material, is over the factor of 103;
nevertheless, the Al concentration could beobtained.

The information of IAEA by INAA (6) also
showed results comparable to the non- correctedvalue in this study. For TORT-1, the correctedvalue in this study seemed to be about 27% lower
than that found by Kratochvil et al. (14) from
INAA, and agreed with the value determined byGraphite
Furnace
AtomicAbsorption
Spectroscopy. For TORT-2, MP, PK and MT, no
information for the Al levels could be found at allin the literatures and the results obtained in thisstudy were novel findings for these materials. For
animal materials, the correction for theconcentration of Si may not be necessary. The
contribution derived from Si is 0.9 %, for example,
for a sample containing 10 ǍgAl/g and 30 ǍgSi/g.
Due to its ease of use and high sensitivity, INAA
has been applied to the determination of Al in
SRMs and CRMs. Even thought animals havemuch lower levels of Al, because of theinterference caused by P which is high animals,
the concentration of Al appeared to be muchhigher in animals than it really has.
REFERENCES
1. Preliminary statistical evaluation of theintercomparison run IAEA-0390, Traceelements in three different level Algae
IAEA-0391/IAEA-0392/IAEA-0393.
IAEA/AL/101P (1998).
2. Intercomparison minor of trace elements in
IAEA Animal Bone (H-5) IAEA. Progress
report No.1 (1982).
3. Parr BM, Intercomparison of minor and traceelements in IAEA Animal Muscle (H-4).
Report No.2, IAEA/RL/69, Vienna (1980).
4. Gladney ES, Elemental concentrations in
NBS biological and environmental standard
reference materials. Anal. Chem. Acta 118,385-396 (1980).
5. NBS Certificates of analysis for SRM-1577a
Bovine Liver, National Bureau of Standards.
Washington D.C. (1982).
6. Muramatsu  Y and Parr RM, Survey ofcurrently available reference materials foruse in connection with the determination of
trace
elements
inbiologicalandenvironmental
materials.
IAEA/RL/128,
Vienna (1985).

- 384 -

3-16

㻝㻠㻞

JAEA-Review 2013-039

7. Intercomparison of Cadmium and otherelements in IAEA Horse-Kidney (H-8) IAEA.
Progress Report No.2 (1985).
8. Lamberty A and Huntau H, The certificationof the mass fraction of As, Cd, Cr, Cu, Hg, Mn,
Pb, Se and Zn in mussel tissue (mytilus
edulis) CRM 278R. European Commission,
Report EUR 18840 EN (1999).
9. Wagstaffe PJ and Griepink B, The
certification of the contents (mass fraction) of
Cd, Pb, As, Hg, Se Cu, Zn, Fe and Mn in threelyophilized animal tissue reference matelials(CRM No 186 Pig Kidney). European
Commission, Report EUR 10618 EN (1986).
10. NIST Certificates of analysis for SRM- 1575a
Trace Elements in Pine Needle, National
Institute of Standards and Technology.
Gaitherburg, MD (2002).
11. Zeiller E, Strachnov V and Dekner R, Reporton the intercomparison run IAEA-155 traceelements in Whey Powder. IAEA/AL/034,
Vienna (1990).
12. Kawamoto K, Sumino, T, Takada J, Tanaka
Y and Akaboshi M, Determination of rareearth and other elements in algae by ICP-MSand neutron activation analysis. J. Radioanal.
Nucl. Chem., 236((1-2), 119-122 (1998).
13. Gladney ES, O’Mailey BT, Roelandts I and
Gills
TE,
Compilationofelemental
concentration data for NBS clinical, biological,
geological and environmental Standard
Reference Materials. NBS Special Publicatio
260-111 (1987).
14. Kratochvil B, Motkosky N, Duke MJM and
Ng D, Determination of trace aluminum
concentration and homogeneity in biologicalreference material TORT-1 by instrumental
neutron activation analysis and graphic
furnace atomic absorption spectroscopy. Can.
J. Chem., 65, 1047-1050 (1987).
ࠊ
15. Schmit JP, Youla M, and Gelinas Y,
Multi-element analysis of biological tissues by
inductively
coupledplasmamass
spectrometry. Anal Chem. Acta, 249(2),495-501 (1991).
16. Dogfish muscle certified reference material
for trace metals and elemental species.
National Research Council Canada (1999).

- 385 -

3-16

㻝㻠㻟

JAEA-Review 2013-039

3-17ᡂ㛗㐣⛬࡟࠾ࡅࡿⴥࡢ⏕య≀㉁୰ࡢ≉ᐃඖ⣲ࡢ࡜ࡾ㎸ࡳ$JURZWKGHSHQGLQJXSWDNHRIVRPHUDUHPHWDOLQWR&OHWKUDFHDHOHDYHV➟ཎ ⱱࠊ㔝▮ ὒ୍ࠊ㛵 ⯆୍
6KLJHUX.DVDKDUD<RXLFKL1R\D .RKLFKLVHNL໭ᾏ㐨኱Ꮫ࢔࢖ࢯࢺ࣮ࣉ⥲ྜࢭࣥࢱ࣮
&HQWUDO,QVWLWXWHRI,VRWRSH6FLHQFH+RNNDLGR8QLYHUVLW\㸯㸬ࡣࡌࡵ࡟

,3 ࡀ㛤Ⓨࡉࢀࠊᨺᑕᛶྠ఩ඖ⣲ࢆ⏝࠸ࡿࣂ࢖ࣜࣙ࢘ࣈ⛉ࡢ᳜≀ࡣ௚ࡢ᳜≀ࡼࡾ୍᱆௨ୖ㧗࠸ࢥࣂࣝࢺ (Co) ྵ᭷ࢆ♧ࡍࠋ௚ࡢ᳜≀ࡣ㖔໬࢜ࢧ࢖࢚ࣥࢫࡢ◊✲ศ㔝࡛ᨺᑕᛶྠ఩ඖ⣲ࡢ᳨ฟ࡟౑⏝ࡉࢀ࡚࠸ࡿࠋ

ᆅᖏ࡜㏻ᖖࡢᅵተ࡜࡛ࢥࣂࣝࢺྵ㔞ࡀ࡯࡜ࢇ࡝

ᡃࠎࡣࠊᖹᡂ㸵ᖺᗘ࠿ࡽࠊࢥࣂࣝࢺࡢ᳜≀యኚࢃࡽ࡞࠸ࡢ࡟ᑐࡋࠊࣜࣙ࢘ࣈࡣᅵተ୰࡟Coࡀ

ෆ࡟࠾ࡅࡿศᕸ≧ែࡸ㞟✚ࡢᶵᗎ࡟ࡘ࠸࡚᫂ࡽ

ከ࠸ሙྜࠊⴭࡋࡃࡇࢀࢆ⃰㞟ࡍࡿᛶ㉁ࡀ࠶ࡿࡇ

࠿࡜ࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡍࡿᮏ◊✲ࢆ㛤ጞࡋࡓࠋ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ[1]ࠋࢥࣂࣝࢺࡀ⏕≀⏺࡟ᬑ㐢ᖹᡂᖺࡲ࡛࡟ࡣࠕ᳜≀ࡢⴥ࡟ྵࡲࢀࡿࢥࣂࣝ

ⓗ࡟Ꮡᅾࡍࡿࡇ࡜ࡣ▱ࡽࢀ࡚࠸ࡿࡀࠊࡑࡢ⃰ᗘࢺศᕸᅗࡢసᡂࠖࠊࠕ᳜≀ࡢⴥ➼࡬ࡢ≉ᐃඖ⣲ࡣపࡃࠊ㝣ୖ᳜≀ࡣ㏻ᖖࠊ஝⇱୰0.1 ppmࡢ࣮࢜ࡢྲྀࡾ㎸ࡳࠖ࡟ࡘ࠸᳨࡚ウࡋࠊࣜࣙ࢘ࣈࡢⴥࠊ

ࢲ࣮࡛࠶ࡿࠋࣜࣙ࢘ࣈࡀCoࢆ⃰㞟ࡍࡿ≉ᛶࡣఱᯞࠊࡉࡃᯝ࡟࠾ࡅࡿ✀ࠎࡢ㔠ᒓࡢศᕸࢆ᫂ࡽ࠿

ࡽ࠿ࡢ⌮⏤ࡀ⪃࠼ࡽࢀ࡞ࡃ࡚ࡣ࡞ࡽ࡞࠸ࠋື≀࡟ࡋ࡚᮶ࡓࠋ

యෆ࡟ࡶࢥࣂࣝࢺࡀᚲせඖ⣲࡜ࡋ࡚ྵࡲࢀ࡚࠾

ࡋ࠿ࡋࠊࡇࡢ◊✲࡛ࡣࠊዃ㞧 ࡍࡿࡑࢀࡒࢀࡢ

ࡾࠊ⏕యᡂศ࡜ࡋ࡚ࢥࣂࣝࢺࢆྵࢇ࡛࠸ࡿࡶࡢ

㔠ᒓᅛ᭷ࡢศᕸࡸ㞟✚ᶵᗎ࡟ࡘ࠸࡚༑ศ᫂ࡽ

࡜ࡋ࡚ࣅࢱ࣑ࣥB 12 ࡀ▱ࡽࢀ࡚࠸ࡿࠋࣜࣙ࢘ࣈࡢ

࠿࡟ࡍࡿ࡟ࡣ⮳ࡗ࡚࠸࡞࠿ࡗࡓࠋ

ᢳฟ≀࡟ࡘ࠸࡚ Euglena (࣑ࢻ࣒ࣜࢩࡢ୍✀) ࠾
ࡼࡧ Ochromonas (㯤㔠Ⰽ⸴ࡢ୍✀) ࢆ⏝࠸ࡓࣂ௒ᅇ ࠊ㸯㸧ள㖄 =Q ࡢᙳ㡪ࢆ༑ศ࡟ྲྀࡾ㝖࠸ࡓࢥࣂࣝ
ࢺࡢ㑅ᢥⓗ⏬ീ໬࢖࢜࢔ࢵࢭ࢖ࡢ⤖ᯝ࡜ᢳฟ≀ࡢ྾཰ࢫ࣌ࢡࢺࣝ
࠿ࡽࠊࣅࢱ࣑ࣥB 12 ࡛ࡣ࡞࠸࡜ࡋ࡞ࡀࡽࡶࠊ㢮⦕㸰㸧ࣜࣙ࢘ࣈࡢᡂ㛗࡟క࠺ྛ✀㔠ᒓ࢖࢜ࣥ✀ࡢ㞟✚ࡢ⤒᫬ⓗኚ໬

య࡛࠶ࡿࢥࣂࣝࢺ࣭࣏ࣝࣇ࢕ࣜࣥ㘒య࡜ࡋ࡚Ꮡ
ᅾࡍࡿࡶࡢ࡜᥎

࡟ࡘ࠸᳨࡚ウࡋࡓࡢ࡛ሗ࿌ࡍࡿࠋ ࡉࢀࡿ࡜ሗ࿌ࡉࢀ࡚࠸ࡿࠋ

ࡋ࠿ࡋ࡞ࡀࡽࢥࣂࣝࢺࡢ᳜≀యෆ࡟࠾ࡅࡿศ

ᮏ◊✲࡟࠾࠸࡚ࠊ⮬↛࡟⏕⫱ࡋ࡚࠸ࡿࣜࣙ࢘

ᕸ≧ែࡸ㞟✚ࡢᶵᗎ࡟ࡘ࠸࡚ࡣࠊࡑࡢᚋ඲ࡃ◊ࣈ࠿ࡽᡃࠎࡣࣜࣙ࢘ࣈࡢⴥࠊ⥲≧ⰼᗎࢆ᥇ྲྀࡋࠊ

✲ࡉࢀ࡚࠸࡞࠿ࡗࡓࠋ㏆ᖺࠊᨺᑕ⥺ࢆ஧ḟඖ⏬

ࡇࢀࢆ஝⇱ᚋࡲࡓࡣ⁐፹ᢳฟἲ࡟ࡼࡾヨᩱࢆసീ࡜ࡋ᳨࡚ฟࡍࡿ࢖࣓࣮ࢪࣥࢢࣉ࣮ࣞࢺ (IP)ࡀ

ᡂࡋࠊᨺᑕ໬࡟௜ࡋࡓࠋࡑࢀࢆ࣐࢞ࣥ⥺ࢫ࣌ࢡ

㛤Ⓨࡉࢀࠊᨺᑕᛶ≀㉁ࡢᖹ㠃ⓗศᕸࡢゎᯒ࡟ᴟࢺ࣓࣮ࣟࢱ࡛ᐃ㔞ࡋࠊIPࢆ⏝࠸⏬ീ໬ࡋࠊඖ⣲ࡵ࡚᭷ຠ࡞ࡶࡢ࡜ࡋ࡚ỗ⏝ࡉࢀࡿࡼ࠺࡟࡞ࡗ࡚

ࡢᐃ㔞ࠊⴥෆศᕸࢆ᫂ࡽ࠿࡟ฟ᮶ࡓࡢ࡛ࠊࡑࢀ

ࡁࡓࠋࢥࣂࣝࢺࡣ୰ᛶᏊ࡟ࡼࡾᐜ᫆࡟ᨺᑕ໬ࡍ

࡟ࡘ࠸࡚ሗ࿌ࡍࡿࠋ

ࡿࡇ࡜ࡀ࡛ࡁࡿࠋࡇࡢᛶ㉁ࢆ฼⏝ࡋ࡚ࢥࣂࣝࢺ
( 60 Co)ࡢIP࡟ࡼࡿⴥෆࡢศᕸࢆ᫂ࡽ࠿࡟ࡋࠊࣜࣙ

㸰㸬ᐇ㦂࢘ࣈࡢ≉␗ⓗ㞟✚ᶵᵓ࡟㛵ࡍࡿᇶ♏ⓗ▱ぢࢆᚓ㸯㸧ᡃࠎࡣࠊࢥࣂࣝࢺࡢ㑅ᢥⓗ⏬ീ໬ࡢࡓࡵ

ࡿࡇ࡜ࢆ┠ⓗ࡟ᮏ◊✲ࢆ㛤ጞࡋࡓࠋࡋ࠿ࡋࠊ㔠࡟ࠊ≀⌮ⓗ๓ฎ⌮ἲ㸦ᨺᑕ⬟ࡢ༙ῶᮇࢆ฼⏝ࡋᒓඖ⣲ࡀ࡝ࡢࡼ࠺࡟ࣜࣙ࢘ࣈ࡟ศᕸࡋ࡚࠸ࡿ࠿

ࡓῶ⾶ฎ⌮㸧࡜໬Ꮫⓗ๓ฎ⌮ἲࢆ⤌ࡳྜࢃࡏࡿ

ࡣ▱ࡽࢀ࡚࠸࡞࠸ࠋ㏆ᖺ࢖࣓࣮ࢪࣥࢢࣉ࣮ࣞࢺ

ࡇ࡜࡟ࡼࡿࠊ㑅ᢥⓗ⏬ീ໬࡟ྲྀࡾ⤌ࢇ࡛ࡁࡓࠋ

-557ࣃ࢖ࣉ ᨺᑕ໬ศᯒ㸦⎔ቃ㸧

- 386 -

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JAEA-Review 2013-039

ࡑࡢ⤖ᯝࢆᖹᡂ㸯㸴ᖺ㸫ᖹᡂ㸯㸶ᖺࡢᡂᯝሗ࿌

ᚲ㡲࡛࠶ࡗࡓࠋࡇࡢࡓࡵࠊ௒ᅇࡣ๓グࡢヨᩱࡢ ᭩࡛ሗ࿌ࡋ࡚࠸ࡿࠋ

=Qࡀ༑ศῶ⾶ࡋࡓ࡜⪃࠼ࡽࢀࡿࠊࡉࡽ࡟㸯㸱㸱ࡇࡢ࡜ࡁࡢ㸮᪥ᚋ㸦⥲ィ㸯㸶㸱㸮᪥ᚋ㸧࡟⏬ീ໬ࡋࡓࠋ⤖ᐃࡣㄪᩚࡉࢀࡓⴥࢆࠊᨺᑕ໬ᚋ

㸳㸮㸮᪥㛫෭༷ࡋࠊ▷༙ῶᮇ᰾✀ࡢᨺᑕ⬟ࡢῶᯝࢆᅗ㸫㸱ࠊᅗ㸫㸲࡟♧ࡍࠋ⾶ࢆᚅࡗ࡚ࠊࣂ࢖࢜࢖࣓࣮ࢪࣥࢢ࢔ࢼࣛ࢖ࢨ࣮

ࢩࢫࢸ࣒㸦ᐩኈࣇ࢕࣒ࣝ..%$6㸧ࢆ⏝࠸࡚㸯㸧ࡢ⤖ᯝ

⾜ࡗࡓࠋᚓࡽࢀࡓ⏬ീࢆᅗ㸫㸯࡟♧ࡍࠋᅗ࠿ࡽ᫂ࡽ࠿࡞ࡼ࠺࡟ࠊ࢝ࣝࢩ࣒࢘ࡣⴥ᯶࡟

ᅗ㸫㸯 

ከࡃࠊள㖄ࡣⴥ᯶ഃࡢⴥ⬦࡟ከࡃࠊࢥࣂࣝࢺࡣ
ⴥࡢ㎶⦕㒊࡟ሢ≧࡟⃰㞟ࡉࢀ࡚࠸ࡿࡇ࡜ࡀ᫂ࡽ
࠿࡜࡞ࡗࡓࠋࢥࣂࣝࢺࡢ⃰㞟ࡀሢ≧࡟࡞ࡗ࡚࠸
ࡿࡇ࡜࠿ࡽࠊⴥࡢ୰࡟ࡣࢥࣂࣝࢺࢆ㞟✚ࡍࡿᾮ⬊ࡢࡼ࠺࡞⤌⧊㸦YDFXROHVSRWVSHFNOHEOR
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᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࡀฟ᮶ࡓ࡜࠸࠺Ⅼ࡛⯆࿡῝࠸࡜⪃࠼࡚࠸ࡿࠋ
ᅗ㸫㸱
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ࡇࡢሙྜࠊ*H༙ᑟయȚ⥺᳨ฟ⿦⨨࡛ࡣ᳨ฟฟ ᅗ㸫㸲

᮶࡞࠸ࠊș⥺ࡢࡳࢆᨺฟࡍࡿ࢝ࣝࢩ࣒࢘ &D ࡟ࡼࡿ㹇㹎࡬ࡢᙳ㡪ࢆ↓ど࡛ࡁ࡞࠸࠿ࡶࡋࢀ࡞࠸
࡜⪃࠼ࠊ࢔࣑ࣝ⟩ࢆ⏝࠸࡚ࠊࡑࡢᙳ㡪ࢆ㝖ཤࡋࡓࡶࡢࡶేグࡋࡓࠋᅗ̿㸰࡟♧ࡍࠋࡇࢀ࡟ࡼࡾࠊⴥ᯶࡟࠾ࡅࡿᙉ࠸ᨺᑕ⬟ࡣș⥺ᨺฟ᰾✀࡟ࡼࡿࡶࡢ࡛࠶ࡿࡇ࡜ࢆ᫂ࡽ࠿࡟ࡍࡿ
ࡇ࡜ࡀ࡛ࡁࡓࠋࡲࡓࠊࢥࣂࣝࢺࡣⴥࡢ࿘㎶࡟㞟✚ࡋ࡚࠸ࡿࡇ࡜ࡶ♧ࡉࢀࡓࠋ

ࡋ࠿ࡋࠊ㸳㸮㸮᪥ࡢ෭༷࡛ࡣࠊඹᏑࡍࡿள㖄㸰㸧ࣜࣙ࢘ࣈࡢᡂ㛗࡟㛵ࢃࡿඖ⣲ࡢኚ໬࡜ⴥࠊ⥲㸦 =Q 7 G㸧ࡢῶ⾶࡛ࡣ༑ศ࡛࡞ࡃࠊࡑࡢ⏬

≧ⰼᗎ࡟ྵࡲࢀࡿ୺せ㔠ᒓ࡛࠶ࡿள㖄 =Q ࠊࢥീ࡬ࡢᙳ㡪ࡀṧᏑࡋ࡚࠸ࡿࡇ࡜ࡶ⪃࠼ࡽࢀࠊࡼ

ࣂࣝࢺ &R ࠊࢭࢩ࣒࢘ &V ࠊࣝࣅࢪ࣒࢘ 5E ࡟ࡾ㛗ᮇ㛫ࡢᨺ⨨࡟ࡼࡿࡑࡢᙳ㡪ࢆ㝖ཤࡋࡓ⏬ീࡘ ࠸࡚ ᳨ウࡍ ࡿࡇ ࡜࡜ࡋ ࡓࠋ ヨᩱࡢ ⴥࠊ ⥲≧ⰼࢆᚓࡿࡇ࡜ࡀࢥࣂࣝࢺࡢศᕸࢆṇࡋࡃ▱ࡿୖ࡛ᗎ ࡣ᥇ ྲྀᚋࡑ ࡢࡲ ࡲ஝⇱ ࡋࡓ ࠋⴥࢆ ᥇ྲྀ ࡍࡿ᫬

3-17- 387 -

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JAEA-Review 2013-039

ᅗ㸫㸶ᮇ ࡣࠊ ⥲≧ⰼ ᗎ࡟ ⰼࡀဏ ࡁጞ ࡵࡿࠊ ᑡࡋ ᡭ๓ࡢ㸵 ᭶࠿ ࡽ㸯㸯 ᭶ࡲ ࡛࡜ࡋ ࡓࠋ ᨺᑕ໬ ࡣ᪥ ᮏཎᏊ

ⴥ
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ຊ◊✲㛤ⓎᶵᵓཎᏊຊ⛉Ꮫ◊✲ᡤ(᪥ᮏཎᏊຊ◊㻠㻜㻜㻜㻚㻜㻜

✲ᡤ)(JRR-㸱)㹑ࣃ࢖ࣉࢆ⏝࠸ࠊ୰ᛶᏊ᮰ᐦᗘ4.3

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♫〇㸧ࢆ⏝࠸࡚⾜ࡗࡓࠋࡑࡢ⤖ᯝࢆZn-65ࡣᅗ㸫㻡㻜㻜㻚㻜㻜
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㸫㸶࡟♧ࡍࠋ㸰㸧ࡢ⤖ᯝᅗ㸫㸳㸪ᅗ㸫㸴ࡢ⤖ᯝ࠿ࡽࠊ㑄⛣㔠ᒓ࡛࠶ࡿᅗ㸫㸳ள㖄㸦Zn-65㸧࠾ࡼࡧࢥࣂࣝࢺ(Co-60)ࡣⴥ࡟ᙉ࠸

ⴥ
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ࢩ࣒࢘(Cs-134)࠾ࡼࡧࣝࣅࢪ࣒࢘(Rb-86)ࡣ⥲≧㻝㻜㻜㻜

ⰼᗎ࡟ከࡃ㞟ࡲࡾࠊ㸶᭶࡞࠸ࡋ㸷᭶ࡲ࡛ࡣ㞟✚

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ࡋ࡚࠸ࡃࡀࠊࡑࢀ௨㝆ࡣ₞ῶࡍࡿഴྥࡀㄆࡵࡽ
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ࢀࡓ㸦ᅗ㸫㸵ࠊᅗ㸫㸶㸧ࠋ᳜≀ࡢ⏕㛗ࡢᚲ㡲ඖ⣲࡛࠶ࡿ࣒࢝ࣜ࢘࡜ྠ᪘

ࡢࣝࣅࢪ࣒࢘࠾ࡼࡧࢭࢩ࣒࢘ࡣᅵተ୰࡟࠾࠸࡚

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㠀ᖖ࡟ప⃰ᗘ࡛Ꮡᅾࡋ࡚࠸ࡿ࡟ࡶ࠿࠿ࢃࡽࡎࠊ

ⴥ⥲≧ⰼᗎ᳜≀࡟ࡼࡗ࡚ᐜ᫆࡟྾཰ࡉࢀ࡚࠸ࡿࡇ࡜ࡀ♧ࡉ

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ࢀࡓࠋள㖄ࠊࢥࣂࣝࢺࡢ㞟✚ᶵᗎࡣ᫂ࡽ࠿࡛࡞

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࠸ࡀᏘ⠇ࡢኚ໬࡜࡜ࡶ࡟ⴥ࡟㞟✚ࡋ࡚࠸ࡿࡢ࡟

㻢㻜㻜ᑐࡋࠊࣝࣅࢪ࣒࢘࠾ࡼࡧࢭࢩ࣒࢘ࡀ᳜≀ࡢᡂ㛗

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࡜㛵ಀࡋ࡚྾཰ࡉࢀࡿ࡜࠸࠺Ⅼ࡛ᑐ⛠ⓗ࡛࠶ࡗ
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ࡓࠋ

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ཧ⪃ᩥ⊩

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[1]Noboru Yamagata,Sadao Murata,Koshu Eiseⴥ⥲≧ⰼᗎ㻯㼟㻙㻝㻟㻠

iinKenkyu Hokoku(1964)13(3)170-5.

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ㅰ㎡

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㻝㻡㻜㻚㻜㻜ࡇ ࡢ ᐇ 㦂 ࡟࠶ ࡓ ࡾ ࠊ ㈗㔜 ࡞ ヨ ᩱ ࢆᥦ ౪ ࡋ ࡚ 㡬㻝㻜㻜㻚㻜㻜㻡㻜㻚㻜㻜࠸ ࡓࠊ ໭ᾏ㐨 ኱Ꮫ ໭᪉⏕ ≀ᅪ ࣇ࢕࣮ ࣝࢻ ⛉Ꮫࢭ

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ࣥ ࢱ࣮ ᳜≀ᅬ ኱㔝  ⚈Ꮚ ᢏ⾡ ᑓ㛛⫋ ဨ࠾ ࡼࡧヨᩱ ㄪᩚ ➼ࡢᢏ ⾡ᣦ ᑟࡋ࡚ 㡬࠸ ࡓࠊ኱ Ꮫඹ ྠ฼⏝㛤ᨺ◊✲ᐊࡢ⃝ᖭ ᾈஅẶࠊᕝᡭ ⛱Ặࠊ▼ᮏ ග᠇Ặ࡟ཌࡃ࠾♩⏦ࡋ࠶ࡆࡲࡍࠋ

- 388 -

3-17

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JAEA-Review 2013-039

3-18
3*$ ࡜ ,1$$ ࡟ࡼࡿᚤᑠ኱Ẽᾋ㐟⢏Ꮚࡢඖ⣲⤌ᡂ ,,(OHPHQWDO&RPSRVLWLRQVRI$WPRVSKHULF6XVSHQGHG3DUWLFXODWH0DWWHUV
E\3*$DQG,1$$ ,, 㤳㒔኱Ꮫᮾி኱Ꮫ㝔⌮ᕤᏛ◊✲⛉ศᏊ≀㉁໬Ꮫᑓᨷ
'HSDUWPHQWRI&KHPLVWU\*UDGXDWH6FKRRORI6FLHQFHDQG(QJQHHULQJ
7RN\R0HWURSROLWDQ8QLYHUVLW\኱ᾆὈႹ㸪ᾏ⪁ཎ඘<DVXML2XUD0LWVXUX(ELKDUD㤳㒔኱Ꮫᮾி㒔ᕷᩍ㣴Ꮫ㒊⌮ᕤᏛ⣔໬Ꮫࢥ࣮ࢫ
'LYLVLRQRI&KHPLVWU\6FKRRORI6FLHQFHDQG(QJLQHHULQJ)DFXOW\RI8UEDQ/LEHUDO$UWV7RN\R0HWURSROLWDQ8QLYHUVLW\ᐩ⏣ᬛஅ㸪Ⳣཎឿ㸪㕥ᮌᬛㄔ
7R\R\XNL7RPLWD6KLJHUX6XJDZDUD7RPRQRUL6X]XNLᮾ໭බ┈ᩥ⛉኱Ꮫ
7RKRNX8QLYHUVLW\RI&RPPXQLW\6HUYLFHDQG6FLHQFH኱ṓᜏᙪ
7VXQHKLNR2WRVKLࡣࡌࡵ࡟≀㉁ࡀྵ᭷࠶ࡿ࠸ࡣ྾╔ࡋ࡚࠸ࡿ㸬ேయ࡟ᙳ㡪ࢆཬ ኱Ẽởᰁࡣᡃࠎࡢ೺ᗣ࡟┤᥋ᙳ㡪ࢆཬࡰࡍࡓࡵ㸪ࡰࡍ໬Ꮫ≀㉁ࡶᑡ࡞ࡃ࡞ࡃ㸪≉࡟┤᥋ⓗ࡞ᙳ㡪ࢆ୚኱ࡁ࡞㛵ᚰ஦࡛࠶ࡿ㸬኱Ẽởᰁ≀㉁ࡢ୍ࡘ࡟኱Ẽᾋ࠼ࡿ࡜⪃࠼ࡽࢀࡿከ⎔ⰾ㤶᪘࡞࡝᭷ᶵ≀㉁ࡢ◊✲ࡀ㐟⢏Ꮚ≧≀㉁ 630 ࡀ࠶ࡿ㸬⢏ᚄࡢᑠࡉ࡞⢏Ꮚࡣ㔜ຊ⢭ຊⓗ࡟⾜࡞ࢃࢀ࡚࠸ࡿ㸬ࡲࡓ㸪᭷ᐖ࡞ඖ⣲ࡶᩘከ࡟ࡼࡿỿ㝆ࡀ㐜ࡃ㸪ࡋࡤࡽࡃ኱Ẽ୰࡟⁻࠸㸪࿧྾࡟ࡃྵࡲࢀ࡚࠾ࡾ㸪⢏Ꮚࡢඖ⣲⤌ᡂࢆ▱ࡿࡇ࡜ࡶ㔜せࡼࡾᡃࠎࡢ⫵ࡢ୰࡟ࡲ࡛฿㐩ࡍࡿ㸬 ᖺ௦ึ㢌㸪࡛࠶ࡿ㸬ࡉࡽ࡟㸪⢏Ꮚࡢ㉳※ࢆゎᯒࡍࡿୖ࡛ࡑࢀࡽ

Ḣ⡿࡛✵ẼືຊᏛⓗ⢏ᚄ μP ࡢ⢏Ꮚ 30 ࡢ኱Ẽࡢඖ⣲⤌ᡂࡣ㔜せ࡞᝟ሗࢆࡶࡓࡽࡍ㸬୰⃰ᗘ࡜ᚰ⫵࡟⑌ᝈࡢ࠶ࡿᝈ⪅ࡢ᪥ูṚஸ⋡࡟┦㛵 ࡑࡇ࡛㸪 ᖺ࠿ࡽᮾிࡢ࣋ࢵࢻࢱ࢘ࣥࡢ୍ࡘ࡛

ࡀ࠶ࡿ࡜࠸࠺␿Ꮫⓗࢹ࣮ࢱࡀሗ࿌ࡉࢀ㸪30 ⢏Ꮚࡢ࠶ࡿከᦶࢽ࣮ࣗࢱ࢘ࣥ࡜ᒣᙧ┴㓇⏣ᕷ࡟࠾࠸࡚㸪ᛶ≧࣭ᣲືࡀὀ┠ࡉࢀ࡚ࡁࡓ㸬ࡉࡽ࡟㸪⢏ᚄࡀࡶࡗ30 ⢏Ꮚࡢ᥇㞟ࢆ࠾ࡇ࡞࠸㸪ඖ⣲⤌ᡂࢆ༶ⓎȚ⥺ศ࡜ᑠࡉ࠸ 30 ⢏Ꮚ⃰ᗘࡣ㸪Ṛஸ⋡࡜ࡢ┦㛵ࡀࡼࡾᯒἲ࡜୰ᛶᏊᨺᑕ໬ศᯒἲ㸪࡞ࡽࡧ࡟ග㔞Ꮚᨺᑕ໬㧗࠸࡜࠸࠺ሗ࿌ࡶ࡞ࡉࢀࡓ㸬ࡑࡢࡓࡵ㸪30 ⢏Ꮚศᯒἲࢆ⏝࠸࡚᫂ࡽ࠿࡟ࡋ࡚ࡁࡓ㸬ᮏ◊✲࡛ࡣ㸪ࡦ࡟㛵ࡍࡿ◊✲ࡀୡ⏺ⓗ࡟┒ࢇ࡟⾜ࢃࢀࡿࡼ࠺࡟࡞ࡗ

ࡁࡘ࡙ࡁࡇࡢ  ᆅⅬ࡛ࡢ 30 ᥇㞟ࢆ⥅⥆ࡍࡿ࡜࡜ࡶ

࡚ࡁࡓ㸬

࡟㸪㒔ᚰ㒊࡜ࡢ኱Ẽ⎔ቃࢆẚ㍑ࡍࡿࡓࡵ࡟㸪ඵ⋤Ꮚ

 630 ࡣ⮬↛άືࡸே㛫άື࡟ࡼࡾᵝࠎ࡞⢏Ꮚࡀ኱ᕷ࡜㸪ᮾி㒔⎔ቃ⛉Ꮫ◊✲ᡤࡢ༠ຊ࡟ࡼࡾᮾி㒔ỤẼ୰࡟ᨺฟࡉࢀ࡚࠸ࡿ㸬ࡇࢀࡽ⢏Ꮚ࡟ࡣከᵝ࡞໬Ꮫᮾ༊࡟࠾࠸࡚ 30 ࡢ᥇㞟ࢆ㛤ጞࡋࡓ㸬ࡇࢀࡽࡢ኱


-55༶Ⓨ࣐࢞ࣥ⥺ศᯒ⿦⨨㸪-5531-55+5-5531-556 ࣃ࢖ࣉ㸪⎔ቃヨᩱᨺᑕ໬ศᯒ

- 389 -

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Ẽ⎔ቃヨᩱࡢඖ⣲⤌ᡂࢆᨺᑕ໬ศᯒἲ࡟࡚ㄪ࡭ࡓ㸬⇇ᑒࡋࡓ㸬ࡇࢀࢆ -556 ࣃ࢖ࣉࡲࡓࡣ -55+5 ࡞ ࠾ 㸪ᮏ ◊ ✲ ࡣ ࢔ ࢪ ࢔ ཎ Ꮚຊ ༠ ຊ ࣇ ࢛ ࣮ ࣒ࣛᏍ࡟࡚  ᫬㛫↷ᑕࡋࡓ㸬෭༷᫬㛫ࢆ࠿࠼࡚ a  ᅇ㸪

)1&$ ࡢ◊✲⅔฼⏝ࢢ࣮ࣝࣉᨺᑕ໬ศᯒࢧࣈࢢ࣮ࣝ

a  ⛊㛫ࣉ࡛ᐇ᪋ࡋࡓ ,1$$ ࡟ࡼࡿ 630 ศᯒࣉࣟࢪ࢙ࢡࢺࡢ᪥

Ꮚࡣ ,1$$ ࡢࡳ⾜࠸㸪3*$ ࡣ⾜ࢃ࡞࠿ࡗࡓ㸬ᮏഃᐇ㦂ࢆ࠿ࡡ࡚⾜ࡗࡓ㸬⤖ᯝ࡜⪃ᐹᐇ㦂᪉ἲ ࡲࡔ㸪᥇㞟ࡋࡓヨᩱࡍ࡭࡚ࡢศᯒࡣ᏶஢ࡋ࡚࠸࡞

 30 ⢏Ꮚࡣ㸪ᮾி㒔ඵ⋤Ꮚᕷࡢ㤳㒔኱Ꮫᮾி༡኱

࠸㸬 ศ㛫↷ᑕ࡟ࡼࡿศᯒࡣ㸪ࡍ࡭࡚ࡢヨᩱ࡟ᑐࡋἑ࢟ࣕࣥࣃࢫ  ྕ㤋ࡢᒇୖ㸪୪ࡧ࡟ᒣᙧ┴㓇⏣ᕷࡢ࡚⾜ࡗࡓࡀ㸪㛗᫬㛫↷ᑕ࡟ࡘ࠸࡚ࡣ㸪ᮾ໭බ┈኱Ꮫᩍ⫱◊✲Ჷࡢᒇୖ࡟࡚⢏ᚄู࡟᥇ྲྀࡋ

࠿࠿ࡿࡓࡵ㸪୍㒊ࡢヨᩱ࡟ࡘ࠸࡚ࡋ࠿⾜࠼࡞࠿ࡗࡓ㸬ࡓ㸬࣏ࣥࣉ࡛኱Ẽࢆ /P ࡢὶ㏿࡛྾ᘬࡋ㸪1,/8ࡲࡓ㸪ࢹ࣮ࢱゎᯒࡶࡍ࡭࡚⤊஢ࡋ࡚࠸࡞࠸ࡓࡵ㸪ࡇࣇ࢕ࣝࢱ࣍ࣝࢲ࣮ࢆ⏝࠸࡚㸪࢖ࣥࣃࢡࢱ࣮ࢆ㏻㐣ࡋࡇ࡛ࡣ㸪30 ⢏Ꮚࡢ▷᫬㛫↷ᑕ࡟ࡼࡿᐃ㔞⤖ᯝࢆࡓ⢏ᚄ ȣP ௨ୗࡢ 30 ⢏ᏊࢆᏍᚄ ȣP ࡜ ȣPሗ࿌ࡍࡿ㸬

ࡢ࣏࣮ࣜ࢝࣎ࢿ࣮ࢺ〇ࣇ࢕ࣝࢱ࡛ศ⢏ࡋ࡚ a ᩘ᪥ 30 ⢏Ꮚࡢ᥇㞟ࡣ㸪 ᖺ࠿ࡽ㸪ඵ⋤Ꮚ࡛ࡣὶ㛫᥇㞟ࡋࡓ㸬᥇㞟ࡣ㸪ඵ⋤Ꮚ࡛ࡣ㝸㐌࡛㸪㓇⏣࡛ࡣ㔞 /PLQ ࡛࢖ࣥࣃࢡࢱ࣮᪉ᘧࢆ⏝࠸࡚㸪Ụᮾ࡛ẖ᭶  ᅇ⾜ࡗࡓ㸬࡞࠾㸪㓇⏣࡛ࡢ᥇㞟ࡣ  ᖺ࡛୰ࡣὶ㔞 /PLQ ࡛ࢧ࢖ࢡࣟࣥ᪉ᘧࢆ⏝࠸࡚ࡣࡌࡵ

Ṇࡋ㸪 ᖺࡣ⾜ࢃ࡞࠿ࡗࡓ㸬ࡓ㸬ὶ㔞ࢆ⮬ືㄪ⠇࡛ࡁ࡞࠸ࡓࡵ㸪ඵ⋤Ꮚ࡛ࡣ㸪᥇  ᖺ  ᭶ࡼࡾ㸪ᮾி㒔Ụᮾ༊ࡢᮾி㒔⎔ቃ⛉Ꮫ㞟ࡉࢀࡓ⢏Ꮚࡀࣇ࢕ࣝࢱ࣮ࡢᏍࢆࡩࡉ࠸࡛࠸ࡁ㸪ࡔ◊✲ᡤࡢᒇୖ࡟࡚ 30 ⢏Ꮚࡢ᥇㞟ࢆ⾜ࡗࡓ㸬ࢧ࢖ࢇࡔࢇὶ㔞ࡀῶᑡࡋ࡚࠸ࡗࡓ㸬᥇㞟ᮇ㛫ࡢᖹᆒὶ㔞

ᐃࢆ⧞ࡾ㏉ࡋࡓ㸬࡞࠾㸪30 ⢏ᐃ࡟᫬㛫ࡀࢡࣟࣥᆺࢧࣥࣉ࣮ࣛ࡟ࡼࡾὶ㏿ /PLQ ࡟࡚኱Ẽࢆ྾ᘬࡋ㸪Ꮝᚄ ȣP ࡢ࣏࣮ࣜ࢝࣎ࢿ࣮ࢺ〇ࣇ࢕ࣝ

50ࢱୖ࡟㸪 ᪥㛫᥇㞟ࡋࡓ㸬ࡲࡓ㸪ඵ⋤Ꮚᕷ࡟࠾࠸࡚

16.7L/minࡓࡔࡋ㸪Ꮝᚄ ȣP ࡢࣇ࢕ࣝࢱࢆ⏝࠸ࡓ㸬 ᥇ྲྀᚋ㸪ࣇ࢕ࣝࢱࢆ⛗㔞ࡋ㸪༙ศ࡟ษ᩿ࡋࡓ㸬∦ࡢ୍ࡘࢆ PP ࡢṇ᪉ᙧ≧࡟ᢡࡾ␚ࡳ㸪)(3 ࣇ࢕࣒ࣝ࡟⇇ᑒࡋ࡚ -55 ༶Ⓨ࣐࢞ࣥ⥺ศᯒ⿦⨨࡟ࡼ

40

3

インパクター法 [μg/m ]6.7L/minࡶ㸪30 ⢏Ꮚ࡜ྠᵝ࡟㸪30 ⢏Ꮚࡢ᥇㞟ࢆ⾜ࡗࡓ㸬

30

20

10

ࡾ⇕୰ᛶᏊࢆ  ᫬㛫↷ᑕࡋ࡞ࡀࡽ㸪༶Ⓨ࣐࢞ࣥ⥺ࢆᐃࡋࡓ㸬ࡑࡢᚋ㸪ྠヨᩱࢆ -5531 ࡲࡓࡣ -55
31 ࡟࡚  ศ㛫↷ᑕࢆ⾜࠸㸪ࡓࡔࡕ࡟  ⛊㛫ᐃࢆ⾜ࡗࡓ㸬෭༷ᚋ㸪ྠヨᩱࢆ࣏ࣜ࢖࣑ࢻ⟩࡜ $O ⟩࡛ໟࡳ㸪 ヨᩱ࡯࡝ࢆࢫࢱࢵࢡୖ࡟ࡋ࡚඲యࢆ▼ⱥ⟶࡟- 390 -

0

0

10

20
30
40
3
サイクロン法 [μg/m ]50

 ! BHFCEI;DBCGH<?A =KDBCGH> < &' *314 =: 8
9K

3-18

㻝㻠㻤

JAEA-Review 2013-039

ࡀ /PLQ ࡟ࡲ࡛࡞ࡿࡇ࡜ࡶ࠶ࡗࡓ㸬୍᪉㸪Ụᮾ࡛ศᕸࢆ⪃៖ࡍࡿ࡜ඵ⋤Ꮚ࡜Ụᮾࡢ㛫࡛ࡢ⢏Ꮚ⃰ᗘ࡟㸪ࡣ㸪ὶ㔞ࡀඵ⋤Ꮚࡼࡾࡶᑡ࡞࠸ࡓࡵ࠿㸪㢧ⴭ࡞ὶ㔞኱ࡁ࡞ᕪࡣࡳࡽࢀ࡞࠿ࡗࡓ㸬a  ᖺࡣ᥇ྲྀ᪉ࡢపୗࡀほࡉࢀ࡞࠸ࡇ࡜ࡢ࡯࠺ࡀከ࠿ࡗࡓ㸬つᐃἲ࡟ၥ㢟ࡀ࠶ࡾ㸪ඵ⋤Ꮚࡢ 30 ⢏Ꮚ⃰ᗘࡣ㐣ᑠホὶ㔞ࡼࡾࡶపୗࡍࡿ࡜㸪᥇㞟ࡉࢀࡓ⢏Ꮚࡢ⢏ᚄࡀ౯ࡉࢀ࡚࠸ࡿ࡜ᛮࢃࢀࡿࡀ㸪ࡇࢀࢆ⪃៖࡟ධࢀࡿ࡜㸪30 ࡜␗࡞ࡗ࡚ࡃࡿ㸬ࡑࡇ࡛㸪Ụᮾ࡟࡚㸪࢖ࣥࣃa  ᖺࡶ  ᖺྠᵝ㸪ඵ⋤Ꮚࡢ᪉ࡀ⢏Ꮚ⃰ࢡࢱ᪉ᘧ࡜ࢧ࢖ࢡࣟࣥ᪉ᘧࡢ  ࡘࡢ᪉ἲ࡛ྠ᫬࡟

ᗘ୰ᚰ್ࡣ㧗࠿ࡗࡓ࡜᥎ᐃࡉࢀࡿ㸬

30 ࡢ᥇㞟ࢆ⾜࠸㸪⢏Ꮚ⃰ᗘࢆẚ㍑ࡋࡓ㸬 /PLQ ࡟ࡼࡿ࢖ࣥࣃࢡࢱ࣮᪉ᘧ࡟ࡼࡿ⢏Ꮚ⃰ ᅗ  ࡟㸪୧᪉ᘧ࡟ࡼࡿ⢏Ꮚ⃰ᗘࢆẚ㍑ࡋࡓ㸬

ᗘࡣ㸪/PLQ ࡟ࡼࡿࢧ࢖ࢡࣟࢺࣟࣥ᪉ᘧ࡜ẚ㍑/PLQ ࡛ࡢ࢖ࣥࣃࢡࢱ࣮᪉ᘧ࡟ࡼࡿ⢏Ꮚ⃰ᗘࡣ⣔⤫ࡋ࡚㸪⣔⤫ⓗ࡟పࡃ࡞ࡗࡓࡀ㸪ඖ⣲⃰ᗘ࡛ࡣྠᵝ࡞ⓗ࡟㸪ࢧ࢖ࢡࣟࣥ᪉ᘧࡼࡾࡶపࡃ࡞ࡗࡓ㸬ࡘࡲࡾ㸪ഴྥࡀほྠࡌ⢏ᚄࡢ⢏Ꮚࡀ᥇㞟ࡉࢀ࡞࠿ࡗࡓ࡜ุ᩿࡛ࡁࡿ㸬ࡢඖ⣲⃰ᗘࡢẚ㍑ࢆ♧ࡍ㸬/PLQ ࡜ /PLQࡉࢀ࡞࠿ࡗࡓ㸬ᅗ  ࡟౛࡜ࡋ࡚ 1D ࡜ 9ࡑࡇ࡛㸪࢖ࣥࣃࢡࢱ࣮᪉ᘧ࡛ࡶ  /PLQ ࡢὶ㔞࡛400

᥇㞟ࢆ⾜ࡗ࡚ࡳࡓ࡜ࡇࢁ㸪ࢧ࢖ࢡࣟࣥ᪉ᘧ࡟ࡼࡿ⢏(a) Naインパクター法 [ng/m ]Ꮚ⃰ᗘ࡜㸪ࡼࡃ୍⮴ࡋࡓ㸬ࡑࡇ࡛㸪 ᖺ࠿ࡽࡣ㸪3ඵ⋤Ꮚ࡛ࡶ㸪/PLQ ࡢὶ㔞࡟ࡼࡿ᥇㞟࡟ኚ᭦ࡋࡓ㸬  ᖺ࡟᥇㞟ࡋࡓ 30 ࡢ⢏Ꮚ⃰ᗘࢆᅗ  D ࡟⟽ࣄࢤᅗ࡛♧ࡋࡓ㸬ཧ⪃࡜ࡋ࡚㸪 ᖺ࠿ࡽ  ᖺ࡟᥇㞟ࡋࡓ 30 ࡢ⢏Ꮚ⃰ᗘࡶᅗ  E ࡟♧ࡋࡓ㸬

インパクター法 16.7 L/min
インパクター法 6.7 L/min

300

200

100

 ᖺ  ᖺ㛫࡛ࡢ⃰ᗘศᕸࡢ୰ᚰ್ࡣ㒔ᚰ࡛࠶ࡿỤ0ᮾࡼࡾࡶ㸪㑹እ࡟఩⨨ࡍࡿඵ⋤Ꮚࡢ᪉ࡀ㧗࠿ࡗࡓࡀ㸪

0

100
200
300
3
サイクロン法 [ng/m ]

400

10
(b) V
(b) 2006年〜2007年

50
3

粒子濃度 [μg/m ]インパクター法 16.7 L/min
インパクター法 6.7 L/min

83(a) 2008年

インパクター法 [ng/m ]

60

40
30

6

4

2
20

0

10
0

八王子

江東

八王子

  " -+"% 

江東



0

2

4
6
8
3
サイクロン法 [ng/m ]10

 # BHFCEI;DBCGH<?A =
KDBCGH> < &' *314 =: 89K
/,/J0.K

3-18- 391 -

㻝㻠㻥

JAEA-Review 2013-039

ࡢ࠶࠸ࡔ࡟᫂░࡞㐪࠸ࡣ㐪࠸ࡣぢࡽࢀࡎ㸪9 ⃰ᗘࡣ㸪ࢀ࡚࠸ࡓࡶࡢ࡜⪃࠼ࡽࢀࡿ㸬⢏Ꮚ⃰ᗘῶᑡࡢཎᅉ࡜

࡝ࡕࡽࡢὶ㔞࡛ࡶ㸪ࢧ࢖ࢡࣟࣥἲ࡜࡯ࡰྠࡌ⃰ᗘࡀ࡞ࡾ㸪ࡇࢀࡽࡢඖ⣲ࢆ࠶ࡲࡾྵࡲ࡞࠸⢏Ꮚࡣఱ࡛࠶

ᚓࡽࢀࡓ㸬⢏Ꮚ⃰ᗘࡢሙྜ࡜▩┪ࡍࡿࡀ㸪ᑡ࡞ࡃ࡜ࡿ࠿⯆࿡ࡀࡶࡓࢀࡿ㸬ࡶᮏ◊✲࡛ᐃ㔞ࡋࡓඖ⣲࡟ࡘ࠸࡚ࡣ㸪ྠ➼࡟᥇㞟ࡉ ඖ⣲⃰ᗘࡣ᥇ྲྀἲ࡟ࡼࡿᕪࡀࡳࡽࢀ࡞࠸ࡓࡵ㸪

Na

1200

Al

700

S

5000

600

1000

4000

200

500

800

3

濃度 [ng/m ]

Mg

250

150

400

100

300

3000

600
400

200

1000

50

200
0

2000

100

八王子

江東

Cl


1600

0

八王子

Ca

300

1400

江東

0

江東

八王子

V

30

0

八王子

Mn


120

250

25

100

200

20

80

150

15

60

100

10

40

50

5

20

江東

1000
800
600
400
200
0

200

0

江東

八王子

Cu

八王子

江東

In

0.12

0

八王子

10

0.08

8

0.06

6

0.04

4

0.02

2

0

八王子

I

12

0.1

江東

江東


150
3

濃度 [ng/m ]3

濃度 [ng/m ]

1200

100

50

0

八王子

0

江東

 $K"

&

6@ "

八王子

(

江東

0


<;:

八王子

江東


89
-+"% =

K

3-18
- 392 -

㻝㻡㻜

JAEA-Review 2013-039

 ᖺ࠿ࡽ  ᖺ࡟᥇㞟ࡋࡓ 30 ࡢඖ⣲⃰ᗘศ

Cl

1400
2006年
1200

ᐃ㔞࡛ࡁࡓ㸬Ụᮾ࡛ࡢ⢏Ꮚ⃰ᗘࡣ㸪ඵ⋤Ꮚࡼࡾࡶప

1000

2008年

3

࠿ࡗࡓࡀ㸪$O࡜ &O ࢆ㝖ࡃඖ⣲⃰ᗘࡣỤᮾ࡛㧗ࡃ㸪

濃度 [ng/m ]ᕸࢆᅗ  ࡟♧ࡍ㸬▷᫬㛫↷ᑕ࡟ࡼࡾ  ඖ⣲ࡢ⃰ᗘࢆ

2007年≉࡟㸪1D㸪0J㸪9㸪0Q㸪&X㸪,Q ࡛ࡢ୰ኸ್ࡣ㸪Ụᮾ

800

600

ࡀඵ⋤Ꮚࡼࡾࡶ⣙  ಸ௨ୖ኱ࡁ࠿ࡗࡓ㸬୍᪉㸪&O ⃰400ᗘࡣ㸪ඵ⋤ᏊࡀỤᮾࡼࡾࡶ⣙  ಸ㧗࠿ࡗࡓ㸬᪥ᮏᾏ

200

12/15-12/16
12/1-12/2
11/17-11/18
11/4-11/5
10/20-10/21
10/6-10/7
9/16-9/17
9/1-9/2
8/20-8/21
8/4-8/5
7/22-7/23
7/9-710
6/16-6/17
6/2-6/3
5/19-5/20
5/7-5/8
4/14-4/15
4/1-4/2
3/18-3/19
3/3-3/4
2/18-2/19
2/4-2/5
1/23-1/24
1/22-1/23
1/21-1/22
12/25-12/26
12/10-12/11
11/26-11/27
11/12-11/13
10/22-10/23
10/9-10/10
9/25-9/26
9/10-9/11
8/27-8/28
8/13-8/14
7/23-7/24
7/9-7/10
6/25-6/26
6/11-6/12
5/28-5/29
5/14-5/15
4/23-4/24
4/9-4/10
3/12-3/13
2/26-2/27
2/13-2/14
1/22-1/23
1/12-1/13
12/11-12/12
11/13-11/14
10/10-10/11
9/28-9/29
8/14-8/15
7/10-7/11
6/12-6/13
5/8-5/9
4/11-4/12
2/13-2/15
1/23-1/27
1/10-1/11

0࡟㠃ࡋ࡚࠸ࡿ㓇⏣࡛ࡣ㸪ᾏሷࡢᙳ㡪࡟ࡼࡾ &O ⃰ᗘࡀ኱ኚ㧗࠸ࡀ㸪࡯࡜ࢇ࡝ࡣ 30 ࡢ⢒⢏࡟ྵࡲࢀ࡚࠾ࡾ㸪  % <57A -+"% = )2 

=



⣽⢏ 30 ࡟࡯ࡰ┦ᙜ ࡛ࡢ &O ⃰ᗘࡣඵ⋤Ꮚࡢ᪉ࡀ

3DUWLFXODWH0DWWHUV$PRQJ6HYHQ$VLDQ&RXQWULHV”⣙  ಸ㧗࠸ࡇ࡜ࡀࡇࢀࡲ࡛ࡢ◊✲ࡼࡾࢃ࠿ࡗ࡚࠸ࡿ㸬

0(ELKDUD<6&KXQJ:&KXHLQWD%)1L7ࡇࡢ㧗⃰ᗘࡣ㸪㒔ᕷᇦ୍࡛⯡࡟ࡳࡽࢀࡿࡶࡢ࡛ࡣ࡞

2WRVKL < 2XUD ) / 6DQWRV ) 6DVDMLPDࡃ㸪ඵ⋤Ꮚ࡟≉᭷࡞≉ᚩ࡛࠶ࡿࡼ࠺࡛࠶ࡿ㸬

6XWLVQD$.%+:RRG-5DGLRDQDO1XFO ዟ⏣ࡽ  ࡣ  ᖺ࡟ᮾி㒔┠㯮༊࡛ 30

&KHP    ࢆ᥇㞟ࡋ㸪ࡑࡢ㔠ᒓᡂศ⃰ᗘࢆሗ࿌ࡋࡓ㸬$O㸪9㸪&X ͇3URJUHVVࡢ ෤ Ꮨ ࡜ ኟ Ꮨ ࡛ ࡢ ᖹ ᆒ ⃰ ᗘ ࡣ ࡑ ࢀ ࡒ ࢀ 㸪 

3DUWLFXODWH0DWWHU$QDO\VLVLQ-DSDQ͇<2XUDRI$WPRVSKHULF

6XVSHQGHG      QJP  ᳨ฟ 㝈 ⏺௨

72WRVKLDQG0(ELKDUD7KH)1&$:RUNVKRSୗ ࡛࠶ࡗࡓ㸬$O ࡣ෤Ꮨ࡛㸪9 ࡣኟᏘ࡛⃰ᗘࡀ㧗࠸࡜

RQWKH8WLOL]DWLRQRI5HVHDUFK5HDFWRUV 

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3KLOLSSLQH ࡉࢀ㸪 ᭶a  ”(OHPHQWDOࡓ㸬 ᭶a  ᭶࡟㧗࠸ 9 ⃰ᗘࡀほ

&RPSRVLWLRQVRI$WPRVSKHULF

᭶࡟ $O ⃰ᗘࡀ㧗࠿ࡗࡓ㸬ඵ⋤Ꮚ࡛ࡶ 9 ࡟ྠᵝ࡞Ꮨ⠇3DUWLFXODWHV &ROOHFWHG LQ -DSDQ IURP  WRኚືࡀほ” < 2XUD + ,JXFKL 7 1DJDKDWD +ࡉࢀࡓ㸬ࡲࡓ㸪ᅗ  ࡟♧ࡍࡼ࠺࡟ &O ࡟᫂░࡞Ꮨ⠇ኚືࡀほࡉࢀ㸪 ᭶a  ᭶࡟㧗⃰ᗘ࡜࡞

1DNDPDWVX72WRVKL0(ELKDUD-5DGLRDQDOࡾ㸪 ᭶a  ᭶ࡣప⃰ᗘ࡛࠶ࡗࡓ㸬ኟᏘࡣẼయ≧࡛ከ

1XFO&KHP   ࡃᏑᅾࡋ㸪෤Ꮨ࡟࡞ࡿ࡜పẼ ͇1$$ DSSOLFDWLRQ WR DLU SDUWLFXODWH PDWWHUࡢࡓࡵ⢏Ꮚୖ࡟จ⦰

ࡍࡿࡢ࡛࠶ࢁ࠺㸬

FROOHFWHG DW WKLUWHHQ VDPSOLQJ VLWHV LQ HLJKW ௒ᚋࡣ㸪㛗᫬㛫↷ᑕ࡟ࡼࡿඖ⣲ࡢᐃ㔞ࢆࡍࡍࡵ㸪$VLDQ FRXQWULHV $ FROODERUDWLYH VWXG\͇ 0㒔ᚰ㒊࡜㑹እᇦ࡟࠾ࡅࡿ 30 ࡢඖ⣲⤌ᡂࡢ≉ᚩࢆ(ELKDUD<6&KXQJ+0'XQJ-+0RRQ%)

᫂ࡽ࠿࡟ࡋ࡚࠸ࡃ㸬

1L72WRVKL<2XUD)/6DQWRV)6DVDMLPD

6XWLVQD%6:HH::LPROZDWWDQDSXQDQG$.

ᡂᯝࡢබ⾲% + :RRG WK ,QWHUQDWLRQDO &RQIHUHQFH RQ

 ”&ROODERUDWLYH 0RQLWRULQJ 6WXG\ RI $LUERQH

0RGHUQ7UHQGVLQ$FWLYDWLRQ$QDO\VLV ඵ

3-18- 393 -

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JAEA-Review 2013-039⋤Ꮚ  ͆7KH3URJUHVVUHSRUWRIHQYLURQPHQWDOVDPSOHDQDO\VLVDQGLWVUHIOHFWLRQWRWKHHQYLURQPHQWDOSURWHFWLRQDXWKRULW\IRUWKHSDVWRQH\HDULQ
-DSDQ͇<2XUD77RPLWD72WRVKLDQG0(ELKDUD 7KH  )1&$ :RUNVKRS RQ WKH8WLOL]DWLRQ RI 5HVHDUFK 5HDFWRUV,QGRQHVLD  ͆$SSOLFDWLRQRI1$$WRDLUSDUWLFXODWHPDWWHUFROOHFWHG DW WKLUWHHQ VDPSOLQJ VLWHV LQ HLJKW$VLDQ FRXQWULHV $ FROODERUDWLYH VWXG\͇ 0
(ELKDUD<6&KXQJ+0'XQJ-+0RRQ%)
1L72WRVKL<2XUD)/6DQWRV)6DVDMLPD6XWLVQD%6:HH::LPROZDWWDQDSXQ$.%
+:RRG-5DGLRDQDO1XFO&KHP 
 

3-18- 394 -

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JAEA-Review 2013-039

3-19
ᾏᡂⅣ㓟ሷ୰ࡢ࣍࢘⣲ࡢ༶Ⓨ࣐࢞ࣥ⥺ศᯒ
3URPSW*DPPDUD\$QDO\VLVRI%RURQLQ0DULQH&DUERQDWHV኱ฟ ⱱࠊ⏣୰೺ኴ㑻
62KGH.7DQDND
⌰⌫኱Ꮫ⌮Ꮫ㒊)DFXOW\RI6FLHQFH8QLYHUVLW\RIWKH5\XN\XVࠊࡣࡌࡵ࡟

ศᯒ࡛ࡣࠊࢧࣥࢦ㦵᱁୰ࡢ࣍࢘⣲ࡢᐃ㔞ࡀ࡛ࡁ࡞ ᮏ◊✲ࡢ┠ⓗࡣࠊⅣ㓟ሷẆ㸦୺ᡂศ㸸&D&2㸧࠸ࠋ⌧ᅾࠊ,&3$(6 ἲࡀࢧࣥࢦࡢ࣍࢘⣲ศᯒ࡟౑୰ࡢ࡛ࡁࡿࡔࡅከࡃࡢඖ⣲ศᯒ࠿ࡽࠊࡑࡢ⏕≀ࡀࢃࢀ࡚࠸ࡿࠋࡑࡢ௚࣍࢘⣲࡟㛵ࡋ࡚᭱㐺࡞ศᯒἲ⏕⫱ࡋ࡚࠸ࡓ⎔ቃỈ࡟ࡘ࠸࡚ࡢ᝟ሗࢆᚓࡿࡇ࡜

ࡀ࠶ࡲࡾ࡞࠸ࠋࡲࡓࠊ༶Ⓨ࣐࢞ࣥ⥺ศᯒࡢࡼ࠺࡟ࠊ

࡛࠶ࡿࠋࡑࡇ࡛ࠊᮏ◊✲࡜ྠ᫬࡟ࠊࢧࣥࢦࡢࣁࣟ

㠀◚ቯ࡛ࡢᐃ㔞ἲࡣࡲࡗࡓࡃࡳ࠶ࡓࡽ࡞࠸ࡢࡀ

ࢤࣥඖ⣲ࡢᨺᑕ໬ศᯒ࡟㛵ࡍࡿ◊✲ࢆ⌧≧࡛࠶ࡿࠋࢧࣥࢦ㦵᱁࡟ࡣࠊ࣍࢘⣲ࡀ⣙ SSP-550 31 ࢆ౑ࡗ࡚⾜ࡗ࡚࠸ࡿࠋ

Ꮡᅾࡍࡿࡢ࡛ࠊཎ◊ࡢ⿦⨨ 3*$ ࢆ౑ࡗ࡚ṇ☜࠿ᾏỈ୰ࡢ࣍࢘⣲࡜ࡑࡢྠ఩య࡟ࡘ࠸࡚ࡣࠊ኱ฟࠊ

ࡘ⢭ᗘࡼ࠸ศᯒࡀྍ⬟࡛࠶ࡿࠋᮏ◊✲࡛ࡣࠊᆅ㉁=XOHJHU㸦㸧࡟ᴫㄝࡋࡓࠋ
࣍࢘⣲ྠ఩య
㸦%%㸧

ㄪᰝᡤࡢࢧࣥࢦᶆ‽ヨᩱ㸦-&S㸧࠾ࡼࡧἈ⦖ࠊ

ࡢྠ఩య஺᥮ࢆ౑ࡗ࡚ࠊSDOHRS+ ࡜࿧ࡤࢀࡿ࢔

࿴ḷᒣࠊࢱ࢖ࠊࣇ࢕ࣜࣆࣥࡢࢧࣥࢦࡢ࣍࢘⣲ྵ㔞࢖ࢹ࢔ࡀࠊ6SLYDFNHWDO  ࡟ࡼࡗ࡚ᥦฟࡉ

ࡢᐃ㔞ࢆ༶Ⓨ࣐࢞ࣥ⥺ศᯒࢆ౑ࡗ࡚⾜ࡗࡓࠋࢀࡓࠋࡍ࡞ࢃࡕࠊᾏᡂࡢ໬▼Ⅳ㓟ሷ㸦㈅Ẇࠊࢧࣥࢦ࡞࡝㸧ࡢ࣍࢘⣲ྠ఩యࡢศᯒ࠿ࡽࠊࡑࢀࡽ⏕≀ࠊࢧࣥࢦヨᩱࡀ⏕ᜥࡋ࡚࠸ࡓ᫬ࡢࠊᾏỈࡢ S+ ࢆ᥎ᐃ࡛ࡁࡿ࡜

Ⅳ㓟ሷᶆ‽࡜ࡋ࡚ᆅ㉁ㄪᰝᡤࡀసᡂࡋࡓ

࠸࠺࢔࢖ࢹ࢔࡛࠶ࡿࠋࡑࡢࡼ࠺࡞ࠊ࣍࢘⣲ྠ఩య

-&S ࢧࣥࢦ ࢆ౑⏝ࡋࡓࠋࢧࣥࢦ㦵᱁ヨᩱࡣἈ࠿ࡽྂ S+ ࢆ᥎ᐃࡍࡿ◊✲ࡢᇶ♏࡜ࡋ࡚ࠊࢧࣥࢦ

⦖㸦ࣝ࢝ࣥ♋ࠊỈ㔩ࠊ༡኱ᮾᓥ㸧ࠊ࿴ḷᒣ㸦ሜ㸧㦵᱁୰ࡢ࣍࢘⣲ྵ㔞ࢆᐃ㔞ࡍࡿࡇ࡜ࡀࠊᮏ◊✲ࡢࢱ࢖㸦࢝ࣥ࢝࢜ᓥ㸧ࠊࣇ࢕ࣜࣆࣥ㸦ࢭࣈᓥ㸧ࡢࢧ┠ⓗ࡛࠶ࡿࠋ

ࣥࢦ♋࠿ࡽ᥇ྲྀࡋࠊ࣑ࣜ࢟ࣗ࢘Ỉ࡛ᩘᅇࠊ㉸㡢Ἴ࢔ࣛࢦࢼ࢖ࢺ㸦&D&2㸧୰࡬ࡢ࣍࢘⣲ࡢඹỿࡀࠊ

Ὑίࡋࠊ஝⇱ࡋ࡚‽ഛࡋࡓࠋ

ࡘࡂࡢ࢖࢜ࣥ஺᥮࡛㉳ࡇࡿ࡜௬ᐃࡍࡿ࡜㸦&D&2

ࠊ༶Ⓨ࣐࢞ࣥ⥺ศᯒ

$ &D$&2㸧㸦$ࡣࠊ࣍࢘㓟࢖࢜ࣥ࡜ࡍࡿ㸧ࠊ ࢧࣥࢦヨᩱ㸦⢊ᮎࡲࡓࡣࣈࣟࢵࢡ≧㸧PJ

ࢧࣥࢦࡢ࣍࢘⣲ྵ㔞ࡣࠊࢧࣥࢦࡀ⏕⫱ࡋࡓᾏỈࡢࢆ࣏ࣜ⿄࡟ᑒධᚋࠊࢸࣇࣟࣥࢩ࣮ࢺ㸦)(3㸧࡟෌Ⅳ㓟࢖࢜ࣥ࡜࣍࢘㓟࢖࢜ࣥࡢẚ࡟ࡼࡗ࡚Ỵᐃࡉᑒධࡋࠊ↷ᑕヨᩱࢆసᡂࡋࡓࠋ࣍࢘⣲ᶆ‽ࡣࠊ

ࢀࡿྍ⬟ᛶࡀ࠶ࡿࠋࡋࡓࡀࡗ࡚ࠊࢧࣥࢦࡢ࣍࢘⣲࠾ࡼࡧ SSP ࣍࢘⣲ࢆྵࡴ࣍࢘㓟ᶆ‽⁐ᾮࢆࢆ ᐃࡍࡿព⩏ࡀ࠶ࡿࠋࡋ࠿ࡋࠊ⇕୰ᛶᏊᨺᑕ໬

ࣟ⣬ୖ࡟ ȣO ሬᕸࡋࠊ஝⇱ࡉࡏࠊࢸࣇࣟࣥࢩ࣮

㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝㹝  ◊✲᪋タ࡜⿦⨨                  ◊✲ศ㔝
-550 3*$ ⎔ቃ໬Ꮫࠊᾏὒᆅ⌫໬Ꮫ- 395 -

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JAEA-Review 2013-039

ࢺ୰࡟ᑒධࡋ࡚సᡂࡋࡓࠋ-550 ࡢ⇕୰ᛶᏊࣅ࣍࢘⣲ྵ㔞ࡣ⾲ ࡟♧ࡍࡼ࠺࡟ࠊ
࡝࠺ࡶSSP

࣮࣒ࢆ౑ࡗ࡚ࠊヨᩱ࡟ࡑࢀࡒࢀࠊ ⛊࠾ࡼࡧࡢ⊃࠸⠊ᅖࡢ್ࢆ♧ࡍࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡾࠊἈ⦖

 ⛊୰ᛶᏊ↷ᑕࡋࠊ༶Ⓨ࣐࢞ࣥ⥺ࢆ ᐃࡋࡓࠋࡢྠࡌࢧࣥࢦ♋ࡢヨᩱ㛫࡛⣙ 㸣ࡢኚືࢆ♧ࡋ

༶Ⓨ࣐࢞ࣥ⥺ࢫ࣌ࢡࢺࣝࢆゎᯒࡋࡓ⤖ᯝࠊࢧࣥࡓࠋୖグࡢ࢖࢜ࣥ஺᥮ᘧࡀࢧࣥࢦࡢ࣍࢘⣲ࡢྲྀࡾࢦヨᩱ୰ࡢ %ࠊ&Dࠊ1D ࡀᐃ㔞ྍ⬟࡛࠶ࡗࡓࠋ࣍

㎸ࡳࢆࢥࣥࢺ࣮ࣟࣝࡋ࡚࠸ࡿࡢ࡛࠶ࢀࡤࠊ⣙ 㸣࢘⣲ࡢ NH9 ༶Ⓨ࣐࢞ࣥ⥺ࣆ࣮ࢡࢆ౑ࡗ࡚ࢧ

ࡢኚືࡣࠊࢧࣥࢦࡀ▼⅊໬ࡋࡓ᫬ࡢࢧࣥࢦ♋ᾏỈࣥࢦ୰ࡢ࣍࢘⣲ࢆᐃ㔞ࡋࡓࠋNH9 ࡢࢼࢺࣜ࢘

୰ࡢⅣ㓟࢖࢜ࣥ࡜࣍࢘㓟࢖࢜ࣥࡢάືᗘẚ㸦⃰ᗘ࣒ࣆ࣮ࢡ࡜࣍࢘⣲ࡢࣆ࣮ࢡࡀ㔜࡞ࡿࡢ࡛ࠊᨺᑕ

ẚ㸧࡜㛵ಀࡋ࡚࠸ࡿ࡜⚾ࡣ᥎ᐃࡋ࡚࠸ࡿࠋࡑࡇ࡛ࠊ

໬ศᯒ࡛ᐃ㔞ࡋࡓࢼࢺ࣒ࣜ࢘ࡢࢹ࣮ࢱ࡜Ⅳ㓟ࢼࢧࣥࢦ♋࡛ ᐃࡋࡓ S+ ࡜ࢧࣥࢦࡢ࣍࢘⣲㔞࡜ࡢࢺ࣒ࣜ࢘ᶆ‽ ⣙ PJ ࢆྠᵝ࡟༶Ⓨ࣐࢞ࣥ⥺ศ㛵ಀ࡟ࡘ࠸࡚⪃ᐹ㐍ࡵ࡚࠸ࡃணᐃ࡛࠶ࡿࠋࡲࡓࠊ

ᯒࡋࡓࢹ࣮ࢱࢆẚ㍑ࡍࡿࡇ࡜࡟ࡼࡗ࡚ࠊࢼࢺࣜ

ᾏእㄪᰝ࡛᥇ྲྀࡋࡓࢧࣥࢦ୰ࡢ࣍࢘⣲ࡢ ᐃ⤖࣒࢘ࣆ࣮ࢡࡢ⿵ṇࢆ⾜ࡗࡓࠋࢧࣥࢦࡢࢼࢺࣜ࢘ᯝࢆ⾲  ࡟ࡲ࡜ࡵࡓࠋ

࣒ྵ㔞ࡣ⣙ SSP ࡛࠶ࡗࡓࠋࢧࣥࢦࡣ࣍࢘⣲ᮏ◊✲࡛ࡣࠊ
≉࡟ࠊࢧࣥࢦ୰ࡢ࣍࢘⣲ྵ㔞࠿ࡽࠊࢆ⣙ SSP ྵࢇ࡛࠸ࡿࡀࠊ⣙ SSP ࡢࢼࢺ࣒ࣜ࢘

ࢧࣥࢦࡀ⏕ᜥࡋ࡚࠸ࡓ⎔ቃỈࡢ໬Ꮫ⤌ᡂࢆ᥎ᐃࡢᐤ୚࡟ࡼࡿ࣐࢖ࢼࢫ⿵ṇࡀᚲせ࡛࠶ࡗࡓࠋᮏ

ࡍࡿࡇ࡜ࢆヨࡳࡓࠋ࣍࢘⣲࡜ྠᵝ࡟ࠊ ౯ࡢ㝜࢖◊✲࡛⏝࠸ࡓ༶Ⓨ࣐࢞ࣥ⥺ศᯒࡢṇ☜ࡉ㸦෌⌧࡛࢜ࣥ࠶ࡿࣇࢵ⣲࡟ࡘ࠸࡚ࠊᾏỈ࠿ࡽ࢔ࣛࢦࢼ

ᛶ㸧ࢆ☜࠿ࡵࡿࡓࡵ࡟ࠊᶆ‽ヨᩱࡢศᯒࢆࡃࡾ

࢖ࢺ࡬ࡢࣇࢵ໬≀࢖࢜ࣥࡢඹỿࡣḟࡢ࢖࢜ࣥ஺

㏉ࡋ⾜ࡗࡓࠋࡇࡢศᯒἲࡢ෌⌧ᛶࡣ 㸣࡛࠶ࡿࠋ᥮཯ᛂᘧ࡟ᚑ࠺ࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿ ,FKLNXQL ࠋ
&D&2 V ) DT  &D) V &2 DT ࠊ⤖ᯝ࡜⪃ᐹࢧࣥࢦᶆ‽ヨᩱ㸦-&S㸹▼ᇉᓥࡢࢧࣥࢦ㸧ࢆ .) >&D)@>&2@>&D&2@>)@ࢧࣥࢦࡢ༶Ⓨ࣐࢞ࣥ⥺ศᯒࡢẚ㍑ᶆ‽࡜ࡋ࡚౑ୖᘧࡣࠊᾏỈࡢࣇࢵ໬≀࢖࢜ࣥ࡜Ⅳ㓟࢖࢜ࣥࡢẚ⏝ࡍࡿࡇ࡜ࡀྍ⬟࠿ࢆ᳨ウࡍࡿ┠ⓗ࡛ࠊᶆ‽ヨᩱࡀࠊⅣ㓟ሷ࡟ඹỿࡍࡿࣇࢵ໬≀࢖࢜ࣥ㔞ࢆࢥࣥࢺࡢศᯒࢆ  ᅇ࡯࡝⧞ࡾ᭰࠼ࡋ༶Ⓨ࣐࢞ࣥ⥺ศᯒ࣮ࣟࣝࡍࡿࡇ࡜ࢆ♧ࡋ࡚࠸ࡿࠋࡉࡽ࡟ࠊᾏỈࡢⅣ

ࡋࡓࠋ-&S ࡢᖹᆒศᯒ್ࡣࠊ r SSP ࡛㓟࢖࢜ࣥࡣࠊS+ ࡜㛵ಀࡍࡿࠋࡋࡓࡀࡗ࡚ࠊᾏỈ࠶ࡗࡓࠋᩥ⊩್ 2NDLHWDO ࡣࠊrࡢ S+ ࠾ࡼࡧ஧㓟໬Ⅳ⣲࡟㛵ࡍࡿ᝟ሗࡀᚓࡽࢀࡿSSP ࡜ሗ࿌ࡉࢀ࡚࠸ࡿࡢ࡛ࠊ㠀ᖖ࡟ࡼ࠸୍⮴ྍ⬟ᛶࡀ࠶ࡿࠋࡑࡇ࡛ࠊࣇࢵ⣲࡜ྠᵝ࡟ࢧࣥࢦẆࢆ♧ࡍࠋ-&S ࡣࠊ▼ᇉᓥ࠿ࡽ᥇ྲྀࡋࡓࣁ࣐ࢧࣥ

ࡢ࣍࢘⣲ࡢṇ☜࡞ᐃ㔞ࡀ㔜せ࡛࠶ࡿࠋࡑࡇ࡛ࠊἈ

ࢦ࠿ࡽసᡂࡉࢀ࡚࠸ࡿࡢ࡛ࠊࢧࣥࢦࡢ࣍࢘⣲ศᯒ⦖㸦ࣝ࢝ࣥ♋ࠊỈ㔩ࠊ༡኱ᮾᓥ㸧ࠊࢱ࢖㸦࢝ࣥ࢝⏝ࡢᶆ‽≀㉁࡜ࡋ࡚᭱㐺࡛࠶ࡿ࡜ᛮࢃࢀࡿࠋ௒ᚋࠊ

࢜ᓥ㸧ࠊࣇ࢕ࣜࣆࣥ㸦ࢭࣈᓥ㸧ࡢࢧࣥࢦ♋࠿ࡽ᥇ศᯒᅇᩘࢆቑࡸࡍ࡞࡝ࡋ࡚ࠊಙ㢗ᛶࡢ㧗࠸ࢹ࣮ࢱྲྀࡋࠊ‽ഛࡋࡓࢧࣥࢦ㦵᱁ヨᩱࡢ༶Ⓨ࣐࢞ࣥ⥺ศࢆᚓࡿࡇ࡜࡟ࡼࡗ࡚ࠊ-&S ࢆ༶Ⓨ࣐࢞ࣥ⥺ศᯒᯒࢆ⾜ࡗࡓ⤖ᯝ㸦ᖹᆒ್㸧ࢆ⾲  ࡟♧ࡍࠋࢧࣥࢦ

ࡢᶆ‽ヨᩱ࡜ࡋ࡚౑⏝ࡋࡓ࠸ࠋ

㦵᱁୰ࡢᖹᆒ࣍࢘⣲ྵ㔞ࡣࢱ࢖ࡢࢧࣥࢦࡀ -55 ࡢ⇕୰ᛶᏊࣅ࣮࣒ࢆ౑࠸ࠊἈ⦖ࡢࢧࣥࢦ

SSP ࡛࠶ࡾࠊࣇ࢕ࣜࣆࣥࡀ SSP ࡛࠶ࡾࠊἈ⦖

ࢆศᯒࡋࡓ⤖ᯝࠊ࣍࢘⣲ࡀ SSP ྵࡲࢀࡿࡀ SSPࠊ࿴ḷᒣࡀ SSP ࡛࠶ࡗࡓࠋࡑ

ࡇ࡜ࡀ᫂ࡽ࠿࡟࡞ࡗࡓ㸦⾲ 㸧ࠋࢧࣥࢦ㦵᱁୰ࡢࡇ࡛ࠊࢧࣥࢦࡀ⏕⫱ࡋ࡚࠸ࡓᾏỈ ᗘ㸦ᖹᆒ್㸧

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JAEA-Review 2013-039

࡜ࢧࣥࢦ㦵᱁୰ࡢ࣍࢘⣲ྵ㔞ࡢ㛵ಀࢆᅗ  ࡟♧ࢵ⣲ྵ㔞࡜ᾏỈ୰ࡢⅣ㓟࢖࢜ࣥ⃰ᗘࡢ㛵ಀ, ᪥ᮏࡍࠋࢭࣈ㸦ࣇ࢕ࣜࣆࣥ㸧ࡢࢹ࣮ࢱࢆ㝖ࡃ࡜ࠊࢧࣥ

ᾏỈᏛ఍ㄅ, 61, 118-122ࢦࡀ⏕⫱ࡋ࡚࠸ࡓᾏࡢᖹᆒỈ ࡣࢱ࢖ࡀ୍␒㧗ࡃࠊ࿴ḷᒣࡀప࠸ࡢ࡛ࠊࢧࣥࢦࡀ⏕⫱ࡋ࡚࠸ࡓ(4)኱ฟⱱ㸦2007㸧ࢧࣥࢦࡢ໬Ꮫീࢆ㏻ࡋ࡚ࡳࡿᾏ

ᗘ࡜࣍࢘⣲ྵ㔞ࡢ㛫࡟ఱ࠿ࠊ㛫᥋ⓗ࡞㛵ಀࡀ࠶ࡿὒ⎔ቃࡢኚ㑄, ᾏὒ໬Ꮫ◊✲, 20, 54-77

ࡶࡢ࡜᥎ᐃࡉࢀࡿࠋ(5) Armid, A., Ohde, S. Shinjo, T., Toki, T. (2008)ࠊ௒ᚋࡢ᪉㔪

Determination of uranium in pore water from coastal᪥ᮏྛᆅࡢࢧࣥࢦࡢ༶Ⓨ࣐࢞ࣥ⥺ศᯒࢆ⾜࠸ࢹ࣮ࢱࢆ⵳✚ࡍࡿ࡜࡜ࡶ࡟ࠊᐇ㦂ᐊ࡛ࡢ࢔ࣛࣞ▼sediment by standard addition ICP-MS analysis. Jour.
Radioanal. Nuclear Chem., 275, 233-237

ྜᡂᐇ㦂ࢆ㏻ࡋ࡚ࠊ࣍࢘⣲ࡢⅣ㓟࢝ࣝࢩ࣒࢘࡬ࡢ
ඹỿ᮲௳ࢆ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࡶ㔜せ࡜⪃࠼ࡿࠋࡲ(6) Hossain, M. S., Ohde, S., Tanaka. K.,ࡓࠊ⌰⌫኱Ꮫ࡟タ⨨ࡉࢀ࡚࠸ࡿ ,&306 ࢆ౑ࡗ࡚ࠊ

Sirirattanachai, S., Snidvongs, A. (2008) Oxygenศᯒࢆ࠾ࡇ࡞ࡗࡓྠࡌࢧࣥࢦヨᩱ࡟ࡘ࠸࡚ࠊ࣍࢘

isotope composition in Porites coral from the Northern⣲ࡢᐃ㔞ࢆ⾜࠺ணᐃ࡛࠶ࡿࠋࡑࡋ࡚ࠊࢹ࣮ࢱࢆẚ

Gulf of Thailand: an implication for its skeletal growth.

㍑᳨ウࡍࡿࠋࡑࡋ࡚ࠊࢧࣥࢦࡀ⏕ᜥࡋ࡚࠸ࡓ⎔ቃ

Bull. Soc. Sea Water Sci., Jpn., 62, 112-113

Ỉࡢ໬Ꮫ⤌ᡂ࡜ࡢ㛵ಀࢆ⪃ᐹࡍࡿணᐃ࡛࠶ࡿࠋ
(7) Bogan, R. A. J., Ohde, S., Arakaki, T., Mori, I.,ࠊᘬ⏝ᩥ⊩

McLeod, C. W. (2009) Changes in rainwater pH

Ichikuni M. Chem. Geol. 27(1979)207.

associated with increasing atmospheric carbon dioxide

Imai N. et al. Geostandard Newslett. 20(1996)165.

after the industrial revolution. Water Air Soil Pollut.,

Ishikawa T., Nakamura E. EPSL 117(1993)567.

196, 263-271

኱ฟⱱ, Zuleger E. ᆅ⌫໬Ꮫ, 33(1999)115
Okai T. et al. Geostandard Newslett. 26(2001)95.

(8) Ohde, S., Tanaka K. (in press) Anthropogenic

Spivack A. J. et al. Nature 363(1993)149.

surfaceᑎᓥ⁠ࡽ, ศᯒ໬Ꮫ 47(1998)451

atmospheric carbon dioxide and its impact on coral

calcification. In Davin T. B. and Brannet A. P., Ed.

ࠊᡂᯝࡢබ⾲

Coral Reefs: Biology, Threats and Restoration, Nova

(1) ኱ฟⱱࠊྜྷᮧ࿴ஂ㸦2006㸧ࠕⅣ㓟ሷࡢᆅ⌫໬Ꮫࠖ࡟ࡼࡏ࡚ࠊᆅ⌫໬Ꮫࠊ40㸪177-178

Sci. Pub., NY

ocean

acidification

withincreasing

3-19(2) Hossain, M. M. M., Ohde, S. (2006) Calcificationof cultured Porites and Fungia under differrent
aragonite saturation state at 25Υ. Proceedings of the10th Coral Reef Symposium, pp. 597-606ᴾ(3) ⏣୰೺ኴ㑻,኱ฟⱱ㸦2007㸧ࢧࣥࢦ㦵᱁୰ࡢࣇ

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JAEA-Review 2013-039

⾲  ᅗ  ୰ࡢࢧࣥࣉࣝࡢ࣍࢘⣲ྵ᭷㔞ࡢᖹᆒ್࡜ᶆ‽೫ᕪ

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ᾏỈ 㻌㻔 㻯㻕     ᅗ  ࢧࣥࢦ㦵᱁୰ࡢ࣍࢘⣲ྵ㔞㸦ᖹᆒ್㸧࡜ᾏỈ ᗘࡢ㛵ಀ U  

3-19

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JAEA-Review 2013-039

3-20᪂ወ࡞ෆໟࣇ࣮ࣛࣞࣥࡢᨺᑕ໬Ꮫⓗᡭἲ࡟ࡼࡿ◊✲Study on the new encapsulated-fullerenes using radiochemical method⟃Ἴ኱Ꮫᩘ⌮≀㉁⛉Ꮫ◊✲⛉ 1࣭㤳㒔኱Ꮫᮾி኱Ꮫ㝔⌮ᕤᏛ◊✲⛉ 2
1
2

Graduate School of Pure and Applied Sciences, University of Tsukuba

Graduate School of Science and Engineering, Tokyo Metropolitan Universityᮎᮌၨ௓ 1࣭ᒾ஭㞝 1࣭⋢⌮⨾ᬛᏊ 1࣭⛅ᒣ࿴ᙪ 2
K. Sueki1, Y. Iwai1, M. Tamari1, K. Akiyama2㏆ᖺࠊࣇ࣮ࣛࣞࣥࡣᶵ⬟ᛶ≀㉁ࡢᮦᩱ࡜ࡋ࡚ᵝࠎ࡞ศ㔝࡛⏝࠸ࡽࢀࡿࡼ࠺࡟࡞ࡗ࡚ࡁ࡚࠸ࡿࠋࡇࡢࣇ
࣮ࣛࣞࣥ࡟㔠ᒓཎᏊࢆෆໟࡋ࡚࠸ࡿ㔠ᒓࣇ࣮ࣛࣞࣥ
ࡣࡑࡢ≉␗࡞ศᏊᵓ㐀࡜㟁Ꮚ≧ែ࠿ࡽ⯆࿡῝࠸≀㉁ࡢ୍ࡘ࡛࠶ࡾ࡞ࡀࡽࠊ⏕ᡂ㔞ࡀ௦⾲ⓗ࡞ࣇ࣮ࣛࣞࣥ
࡛࠶ࡿ C60 ࡟ẚ࡭ 1/1000 ௨ୗ࡜㠀ᖖ࡟ᑡ࡞࠸ࡓࡵࠊ
༑ศ࡞◊✲ࡀ㐍ᒎࡋ࡚࠸ࡿ࡜ࡣゝ࠼࡞࠸≧ែ࡟࠶ࡿࠋ
ࡇࡢࡼ࠺࡞ᑡ㔞ࡢ≀㉁ࡢᛶ㉁ࢆㄪ࡭ࡿୖ࡛ࠊヨᩱ࠿ࡽᨺฟࡉࢀࡿᨺᑕ⥺ࢆ᳨ฟᡭẁ࡜ࡍࡿࣛࢪ࢜ࢡ࣐ࣟ
ࢺࢢࣛࣇ࢕࣮ࡣ㠀ᖖ࡟᭷ຠ࡞ᡭẁ࡛࠶ࡿ࡜ゝ࠼ࡿࠋࡲࡓࠊȖ ⥺ࢆࣔࢽࢱ࡟⏝࠸ࡿࣛࢪ࢜ࢡ࣐ࣟࢺࢢࣛࣇ
࢕࣮࡛ࡣ௚ඖ⣲ྠ᫬࡟ศᯒࡀྍ⬟࡛࠶ࡾࠊ㔠ᒓࣇ࣮ࣛࣞࣥࢆศᯒᑐ㇟࡜ࡍࡿሙྜࡣෆໟ㔠ᒓࡈ࡜ࡢᛶ㉁ࡢ㐪࠸ࢆྠ᫬࡟ㄪ࡭ࡿࡇ࡜ࡀ࡛ࡁࡿࠋࡲࡓࠊᨺᑕᛶ
ྠ఩యࢆෆໟࡋࡓࣇ࣮ࣛࣞࣥࡣࡑࢀ⮬యࡀ᪂ࡋ࠸ᶵ
⬟ࢆ᭷ࡍࡿ≀㉁࡛࠶ࡾࠊỈ⁐ᛶࡢศᏊࢆྜᡂࡍࡿࡇ
࡜࡟ࡼࡗ࡚᪂ࡓ࡞ᛂ⏝࡬ࡢⓎᒎᛶࢆࡶࡓࡽࡍ࡜⪃࠼ࡽࢀࡿࠋᮏ◊✲࡛ࡣࣛࣥࢱࣀ࢖ࢻ㔠ᒓෆໟࣇ࣮ࣛࣞࣥࡢศ
Ꮚෆࡢ཮ᴟᏊ࣮࣓ࣔࣥࢺࡢ⣔⤫ⓗ◊✲࡜Ỉ㓟ᇶࢆᑟධࡍࡿ㐣⛬࡟ࡘ࠸࡚ཎᏊ⅔࡛୰ᛶᏊᨺᑕ໬ࡋࡓࢺࣞ
࣮ࢧ࣮ࢆ⏝࠸࡚◊✲ࡋࡓࠋ㸯㸬ࣛࣥࢱࣀ࢖ࢻ㔠ᒓࣇ࣮ࣛࣞࣥࡢ཮ᴟᏊ࣮࣓ࣔࣥ
ࢺ࡟㛵ࡍࡿ◊✲࡟ࡘ࠸࡚
La, Ce, Pr, Nd, Gd ࢆෆໟࡋࡓ M@C82 ࡣࢣ࣮ࢪࢆᵓ
ᡂࡍࡿ C82 ࣇ࣮ࣛࣞࣥࡢᵓ㐀ࠊෆໟ㔠ᒓཎᏊ࠿ࡽࢣ
࣮ࢪ࡬ࡢ㟁Ⲵ⛣ືᩘ࡞࡝㟁Ꮚ≧ែࡀ஫࠸࡟㠀ᖖ࡟㢮ఝࡋࡓ໬ྜ≀࡛࠶ࡿࠋᐇ㝿ࠊ໬ྜ≀ࡢ㟁Ꮚ≧ែࢆㄪ࡭ࡿᡭẁࡢ୍ࡘ࡛࠶ࡿ⣸እྍど㏆㉥እ྾཰ࢫ࣌ࢡࢺࣝ ᐃ࡛ࡣࠊ஫࠸࡟㠀ᖖ࡟㢮ఝࡋࡓࢫ࣌ࢡࢺࣝࢆ♧ࡍࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿࠋ[1] ࡋ࠿ࡋ࡞ࡀࡽ୍᪉࡛ࣆ
ࣞࢽࣝᅛᐃ┦ࢆᣢࡘࣇ࣮ࣛࣞࣥศྲྀ⏝࣒࡛࢝ࣛ࠶ࡿ
Buckyprep ࣒࢝ࣛ࡟࠾ࡅࡿࡇࢀࡽ M@C82 ࡢಖᣢ᫬㛫ࡣⱝᖸ␗࡞ࡗ࡚࠾ࡾࠊෆໟࡉࢀࡓ㔠ᒓཎᏊ࡟ࡼࡾࠊ

ᅛᐃ┦࡜┦஫స⏝ࡍࡿࣇ࣮ࣛࣞࣥࢣ࣮ࢪ⾲㠃ࡢᛶ㉁࡟ⱝᖸࡢኚ໬ࢆࡶࡓࡽࡍࡇ࡜ࢆ♧၀ࡋ࡚࠸ࡿࠋᮏ◊✲࡛ࡣࠊ㔠ᒓෆໟࣇ࣮ࣛࣞࣥ M@C82㸦M = LaࠊCeࠊPrࠊNdࠊGd㸧ࡢࣆࣞࢽࣝᅛᐃ┦(Buckyprep ࣒࢝ࣛ)࡟࠾ࡅࡿಖᣢ᫬㛫ࢆ⢭ᐦ࡟ ᐃࡋࠊෆໟ㔠ᒓཎᏊ࡟ࡼࡿ M@C82 ࡢᛶ㉁ࡢ㐪࠸ࢆ᫂ࡽ࠿࡟ࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡋࡓࠋᐇ㦂ࡣ㔠ᒓෆໟࣇ࣮ࣛࣞࣥࡢྜᡂࡣ࢔࣮ࢡᨺ㟁ἲࢆ⏝࠸࡚⾜ࡗࡓࠋ࢔࣮ࢡᨺ㟁࡟⏝࠸ࡓⅣ⣲㟁ᴟࡣ 5✀㢮ࡢࣛࣥࢱࣀ࢖ࢻࡢ㔠ᒓ㓟໬≀㸦La2O3ࠊCeO2ࠊ
Pr6O11ࠊNd2O3ࠊGd2O3㸧ࢆΰྜࡋࡓ⢊ᮎ࡜ࢢࣛࣇ
࢓࢖ࢺ⢊ᮎ࡜ࢆཎᏊẚ࡟ࡋ࡚㔠ᒓ㸸Ⅳ⣲=1:50 ࡜࡞ࡿࡼ࠺࡟ΰࡐࠊ10 Imm × 100 mm ࡟ᙧᡂࡋࠊ
1000 Υ࡟࡚↝⤖ࡋ࡚సᡂࡋࡓࠋࡇࡢⅣ⣲Წࢆ⏝࠸
࡚ He 㞺ᅖẼࠊᅽຊ 500 Torrࠊ┤ὶ㟁ὶ 50 A ࡢ᮲௳࡛࢔࣮ࢡᨺ㟁ࢆ⾜࠸ࠊ㔠ᒓࣇ࣮ࣛࣞࣥࢆྵࡴࢫࢫ
ࢆྜᡂࡋࡓࠋࡇࡢࢫࢫࡼࡾ 1,2,4-ࢺࣜࢡࣟࣟ࣋ࣥࢮ
ࣥࢆ⏝࠸ࡓ㑏ὶࢆ 8 ᫬㛫⾜࠸ࠊࣇ࣮ࣛࣞࣥᡂศࡢᢳ
ฟࢆ⾜ࡗࡓࠋࡇࡢᢳฟ⁐ᾮ࠿ࡽ࣓ࣥࣈࣞࣥࣇ࢕ࣝࢱ
࣮ࢆ⏝࠸࡚୙⁐ᡂศࢆ㝖ཤࡋࠊ⁐ᾮࢆ஝ᅛࡋࡓࡶࡢ
ࢆ⇕୰ᛶᏊ↷ᑕ⏝ࡢヨᩱ࡜ࡋࡓࠋࡇࡢヨᩱࢆ㧗⣧ᗘ▼ ⱥ ⟶୰ ࡟ᑒ ධ ࡋࠊ ᪥ᮏ ཎ Ꮚຊ ◊✲ 㛤 Ⓨᶵ ᵓࡢ
JRR-3M Ỉຊ↷ᑕタഛ HR-1 Ꮝ㸦flux: 9.6×1013
n/cm2 㺃 sec 㸧 ཬ ࡧ Ẽ ㏦ ⟶ ↷ ᑕ タ ഛ PN-1 㸦 flux:
5.2×1013 n/cm2㺃sec㸧࡟࠾࠸࡚⇕୰ᛶᏊ↷ᑕࢆࡑࢀࡒࢀ 6 ᫬㛫ཬࡧ 20 ศ㛫⾜࠸ࠊヨᩱࢆᨺᑕ໬ࡋࡓࠋ
ᨺᑕ໬ࡋࡓヨᩱࡣ㛤ᑒᚋࠊࡍࡳࡸ࠿࡟ CS2 ࡟⁐ゎࡋࠊ࣓ࣥࣈࣞࣥࣇ࢕ࣝࢱ࣮࡛⇕୰ᛶᏊ↷ᑕ୰࡟⏕ࡌࡓ୙⁐ᡂศࢆ㝖ཤࡋࡓࠋࡇࡢࢁᾮࢆ஝ᅛࡋࡓᚋࠊࢺ࢚ࣝ
ࣥ 1mL ࡟෌⁐ゎࡋ࡚ HPLC ᒎ㛤⏝ࡢヨᩱ࡜ࡋࡓࠋ
HPLC ศᯒ࡟ࡣ Agilent-1200LC ࢩࢫࢸ࣒ࢆ⏝࠸ࠊᅛᐃ┦࡜ࡋ࡚ Pyrenyl ᅛᐃ┦ࢆࡶࡗࡓ Buckyprep࣒࢝ࣛࢆ⏝࠸ࡓࠋヨᩱࡣᒎ㛤ᾮ࡜ࡋ࡚ࢺ࢚ࣝࣥࢆ⏝࠸ࠊflow rate: 3.2 mL/minࠊSample Volume㸸1 mLࠊᗘ㸸ᐊ ࡢ᮲௳࡛ HPLC ᒎ㛤ࡋࠊ⁐ฟᡂศࢆ 20

JRR-3M PN-1, JRR-4 T-ࣃ࢖ࣉ, ᨺᑕ໬Ꮫ- 399 -

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JAEA-Review 2013-039⛊ࡈ࡜࡟ศ⏬ࡋࡓࠋࡇࡢศ⏬ࡋࡓᡂศࡼࡾᨺฟࡉࢀ
ࡿJ⥺ࢆ㧗⣧ᗘ Ge ༙ᑟయ᳨ฟჾ࡟࡚ ᐃࡋࠊྛM@C82 ᡂศࡢಖᣢ᫬㛫ࢆㄪ࡭ࡓࠋ
⤖ᯝࡣࠊᅗ 1 ࡟ La, Ce, Pr, Nd, Gd ࢆෆໟࡋࡓ
M@C82 ࡢ HPLC ⁐㞳᭤⥺ࢆ♧ࡋ࡚࠸ࡿࠋLa ࡟ࡘ࠸࡚ࡣ PN-1 Ꮝ࡟࠾࠸࡚↷ᑕࡋࡓヨᩱࢆࠊCeࠊPrࠊNdࠊ
Gd ࡟ࡘ࠸࡚ࡣ HR-1 Ꮝ࡟࠾࠸࡚↷ᑕࡋࡓヨᩱ࠿ࡽᚓࡽࢀࡓࢹ࣮ࢱࢆᇶ࡟సᡂࡋ࡚࠶ࡿࠋPN-1ࠊHR-1 ྛ↷ᑕ࡟࠾ࡅࡿಖᣢ᫬㛫ࡣ Ce ࡢಖᣢ᫬㛫࡜ UV ࡟ࡼࡾࣔࢽࢱࡋࡓ✵ࣇ࣮ࣛࣞࣥࡢಖᣢ᫬㛫࠿ࡽ⿵ṇࡋࡓࠋᚓࡽࢀࡓ⁐㞳᭤⥺ࢆḟ࡟♧ࡍ Extreme ࣔࢹࣝ࡟ࡼࡾ
ࣆ࣮ࢡࣇ࢕ࢵࢸ࢕ࣥࢢࢆ⾜࠸ࠊྛ M@C82 ࡢಖᣢ᫬㛫ࢆồࡵࡓࠋ
Extreme ࣔࢹࣝ:

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㻾㼑㼠㼑㼚㼠㼕㼛㼚㻌㼀㼕㼙㼑㻌㻛㻌㼙㼕㼚ᅗ 1㸬M@C82 ࡢࣆࣞࢽࣝᅛᐃ┦㸦Buckyprep ࣒࢝ࣛ㸧࡟࠾ࡅࡿ HPLC ⁐㞳ᣲື㸸HPLC ᒎ㛤᮲௳ࡣ
ヨᩱయ✚: 1 mLࠊὶ㏿: 3.2 mL/minࠊᒎ㛤 ᗘ: 20Υ࡛࠶ࡗࡓࠋ⾲ 1. M@C82 ࡢ HPLC ಖᣢ᫬㛫
M@C82ಖᣢ᫬㛫 / min
La
Ce
Pr
Nd
Gd

60.13 ± 0.03
60.88 ± 0.04
60.98 ± 0.05
61.00 ± 0.03
62.22 ± 0.07

ヲ⣽࡞཮ᴟᏊ࣮࣓ࣔࣥࢺ࡟ࡘ࠸࡚ࡢ㆟ㄽ࠾ࡼࡧศᏊ
ᵓ㐀࡟ࡘ࠸࡚ࡣ௒ᚋ᳨ウࡋ࡚⾜ࡃணᐃ࡛࠶ࡿࠋ
㸰㸬Ỉ⁐ᛶࣛࣥࢱࣀ࢖ࢻ㔠ᒓࣇ࣮ࣛࣞࣥࡢྜᡂ࡟ࡘ
࠸࡚ࣇ࣮ࣛࣞࣥ㢮ࡣࡑࢀࡔࡅ࡛ࡣỈ࡟୙せ࡛࠶ࡿࡀࠊ
ㄏᑟయࢆ໬Ꮫಟ㣭ࡍࡿࡇ࡜࡟ࡼࡗ࡚Ỉ⁐ᛶ࡟࡞ࡾ⏕య࡞࡝࡬ࡢྲྀࡾ㎸ࡳࡀྍ⬟࡟࡞ࡿࠋࡲࡓಟ㣭ࡍࡿㄏᑟయࢆኚ࠼ࡿࡇ࡜࡛ࠊ⏕యෆࡢ௵ពࡢ⮚ჾ࡞࡝࡟ྠ
ࣇ࣮ࣛࣞࣥࢆㄏᑟ࣭จ⦰ࡍࡿࡇ࡜ࡀྍ⬟࡟࡞ࡿࠋࣇ
࣮ࣛࣞࣥࢣ࣮ࢪ࡟ࡣඖ⣲ࡢෆໟࡀྍ⬟࡛࠶ࡾࠊෆໟ
ࡉࢀࡿඖ⣲ࢆᨺᑕᛶྠ఩ඖ⣲࡟ࡍࡿࡇ࡜࡛ࠊ㧗ឤᗘᨺᑕ⥺ ᐃࢆྍ⬟࡜ࡍࡿᶵ⬟ᛶ≀㉁ࡢྜᡂ࠶ࡿ࠸ࡣ
ෆໟࡋࡓᨺᑕᛶྠ఩ඖ⣲࠿ࡽࡢᨺᑕ⥺ࢆ฼⏝ࡋࡓデ᩿⸆࡞࡝࡬ࡢᛂ⏝ࡀᮇᚅ࡛ࡁࡿࠋ ࡑࡇ࡛᪤Ꮡࡢࣛࣥࢱࣀ࢖ࢻ㔠ᒓࣇ࣮ࣛࣞࣥࢆ୰ᛶ
Ꮚᨺᑕ໬ࡋ࡚ᚓࡽࢀࡓᨺᑕᛶྠ఩ඖ⣲ෆໟࣇ࣮ࣛࣞ
ࣥ໬Ꮫಟ㣭ࡍࡿᐇ㦂ࢆ᳨ウࡋࡓࠋ La ࠾ࡼࡧ Sm 㔠ᒓࣇ࣮ࣛࣞࣥࢆྵࡴ⛒ᢳฟ≀ࢆ
ཎᏊ⅔࡛୰ᛶᏊ↷ᑕࡋࡓࠋCS2 ⁐፹࡛⁐ゎࡋࡓᚋ࡟
0.2ȣm ࡢࣇ࢕ࣝࢱ࣮ࢆ⏝࠸࡚ࢁ㐣ࡋࠊ⁐፹ࢆࢺ࢚ࣝ
ࣥ࡟⨨ࡁ᥮࠼ࡓࠋBuckyprep ᅛᐃ┦ࢆ⏝࠸ࡓ HPLCᒎ㛤ࢆ⾜࠸ 140La@C82 ࠾ࡼࡧ 153Sm@C82 ࢆศ⏬ࡋࡓࠋࡇࡢヨᩱ࡟ C60 ࢆ 1 mg ຍ࠼ࠊࡉࡽ࡟ࢺ࢚ࣝࣥ⁐ᾮ
2.5ml ࡋ ࡓ ࠋ ࡇ ࡇ ࡟ 㣬 ࿴ KOH Ỉ ⁐ ᾮ 1ml ࡜
TBAH10%⁐ᾮ 3 ⁲ࢆຍ࠼࡚⃭ࡋࡃ᣺࡜࠺ࡉࡏ࡚໬
Ꮫ཯ᛂࢆ㉳ࡇࡉࡏࡓࠋ᣺࡜࠺᫬㛫ࡢ㐪࠸࡟ࡼࡿࢺࣝ
࢚ࣥ⁐ᾮཬࡧ࢔ࣝ࢝ࣜ⁐ᾮࡉࡽ࡟୙⁐ᛶᡂศ࡟࠾ࡅ
ࡿ 140La ࠾ࡼࡧ 153Sm ࡢᨺᑕ⬟ศᕸࠊ୙⁐ᛶᡂศࢆ⵨␃Ỉ࡛⁐ゎࡋࡓࡢࡕ࡟ࢧ࢖ࢬ᤼㝖ࢤࣝࢡ࣐ࣟࢺ࢝
࣒ࣛࢆ⏝࠸࡚࢔ࣝ࢝ࣜ࢖࢜ࣥ࡞࡝࠿ࡽศ㞳ࡋࠊᨺᑕᛶྠ఩యෆໟࣇࣛࣞࣀ࣮ࣝࡢ཰⋡࡞࡝ࢆㄪ࡭
ࡓࠋ&࡟7%$+ࢆゐ፹࡟ࡋ࡚.2+ࢆ཯ᛂࡉࡏࡿ࡜
& 2+ ;ࡀྜᡂࡉࢀࡿ>@ࠋྠᵝࡢᡭἲ࡟ࡼࡾ/D㸾&࠾ࡼࡧ6P#&࠿ࡽ5,㸾& 2+ ;ࢆྜᡂࡉࡏࡓࠋ
ࡑࢀࡒࢀࡢ5,࠿ࡽࡢ࣐࢞ࣥ⥺ࢆ⏝࠸࡚཯ᛂࡉࡏࡿࡓ
ࡵࡢ᣺࡜࠺᫬㛫ࢆኚ໬ࡉࡏࡓ᫬ࡢỈ⁐ᛶ⏕ᡂ≀ࡢ཰⋡ࢆồࡵࡓࠋᙜึࠊࢺ࢚ࣝࣥ┦࡟Ꮡᅾࡋ࡚࠸ࡓ5,ࡣ㣬࿴.2+Ỉ⁐ᾮ࡜7%$+ࢆ཯ᛂࡉࡏࡿ࡜ࡍࡄ࡟Ỉ┦ഃ࡜ࢺ࢚ࣝࣥ࡜Ỉ⁐ᾮࡢ㛫࡟ⲔⰍࡢ୙⁐ᛶᡂศ࡬࡜
⛣ືࡍࡿࠋࡇࡢኚ໬ࡣࢺ࢚ࣝࣥ┦࡟⁐ࡅ࡚࠸ࡿ⣸Ⰽ
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⮴ࡋ࡚࠸ࡿࠋࡇࢀࡽࡢ┦࡬ࡢ⛣ື㔞ࢆᅗ㸰࡟♧ࡍࠋ᣺࡜࠺᫬㛫ศ࡛ࡣ㞴⁐≀࡟㸶㸮㸣Ꮡᅾࡋ࡚࠸ࡿ
ࡀ᣺࡜࠺᫬㛫ࢆ᫬㛫࡟ࡍࡿ࡜ࡑࡢᡂศࡣ㸴㸮㸣⛬ᗘ࡟࡞ࡾࠊ.2+Ỉ⁐ᾮ┦࡟⁐ゎࡍࡿ๭ྜࡀୖ᪼ࡋࡓࠋ
ࡲࡓࠊ㞴⁐≀࡟⵨␃Ỉࢆຍ࠼ࡿ࡜⁐ゎࡍࡿࡀࠊࡇࡢ
⁐ᾮࢆࢧ࢖ࢬ᤼㝖ࢤࣝࢡ࣐ࣟࢺ࣒࢝ࣛ࡟㏻ࡋ࡚࢔ࣝ
࢝ࣜ࢖࢜ࣥ࡞࡝࠿ࡽศ㞳ࡍࡿࠋࡇࢀ࡟ࡘ࠸࡚ࡶ 5,࠿ࡽࡢ࣐࢞ࣥ⥺࡟ࡼࡗ࡚཰⋡ࢆồࡵࡓࠋ᣺࡜࠺᫬㛫࡟ࡼࡿኚ໬ࢆᅗ㸱࡟♧ࡍࠋ⁐ฟ఩⨨㸰㸯㸴㸮⁲ࡣศᏊࢧ࢖ࢬࡀ኱ࡁ࡞ 5,㸾& 2+ ;ࡀ⁐ฟࡋ࡚࠸ࡿࠊࡇ
ࢀ࡟ᑐࡋ࡚㸴㸯㸯㸮㸮⁲ࡣศᏊࢧ࢖ࢬࡢᑠࡉ࡞࢖
࢜ࣥ࡞࡝ࡀ⁐ฟࡋ࡚࠸ࡿࠋ㸰㸯㸴㸮⁲ࡢࣇࣛࢡࢩࣙ

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JAEA-Review 2013-039

࡛ࣥࡣ᣺࡜࠺᫬㛫㸯㸮ศ࡛ࡣ཰⋡ࡀ㸲㸮㸣࡛࠶ࡿࡀ᣺࡜࠺᫬㛫㸶᫬㛫࡟࡞ࡿ࡜㸴㸮㸣ࡲ࡛ୖ᪼ࡋ࡚࠸ࡿࠋ
ࡲࡓࠊ㸴㸯㸯㸮㸮⁲ࡢࣇࣛࢡࢩࣙࣥ࡟ࡣᨺᑕ⥺ࡣ࡯
࡜ࢇ࡝ほ ࡉࢀ࡚࠸࡞࠸ࠋ௒ᅇ᣺࡜࠺᫬㛫ࢆ㸯㸮ศ࠿ࡽ㸶᫬㛫ࡲ࡛ኚ໬ࡉࡏ࡚⏕ᡂ≀ࡢ཰⋡ኚ໬࡞࡝ࢆ
ㄪ࡭ࡓࡀ཯ᛂ᫬㛫ࡀ▷࠸ሙྜ࡟㸱┦࡟ศ㞳ࡍࡿ࠺ࡕࡢ㞴⁐ᡂศ࡟㸶㸮㸣Ꮡᅾࡋࠊࡑࡢᡂศࢆ⵨␃Ỉ࡛⁐࠿ࡋ࡚࣒࢝ࣛศ㞳ࡍࡿ࡜࣒࢝ࣛࡢᅛᐃ┦࡟྾╔ࡍࡿᡂศࡀᏑᅾࡍࡿࡇ࡜ࡀࢃ࠿ࡗࡓࠋࡇࢀࡽࡢᡂศࡣ 2+ࡀ༑ศ࡟௜ຍࡋ࡚࠸࡞࠸ࡔࡅ࡛ࡣ࡞ࡃࢤࣝ࡟ᑐࡋ࡚
྾╔ࡍࡿࡼ࠺࡞཯ᛂᛶࢆᣢࡗ࡚࠸ࡿࡇ࡜ࡀ᥎ᐃࡉࢀ
ࡿࠋࡇࢀࡽࡢࡇ࡜࠿ࡽ཯ᛂ᫬㛫ࡣ㸯᫬㛫௨ୖࡀᚲせ࡛࠶ࡿࡇ࡜ࡀࢃ࠿ࡗࡓࠋ

1
140

La@C82㻌
Sm@C82153

Sm 21-60
La 21-60

0.8

Sm 61-100
La 61-100

0.6

0.4

1
140
153

La@C82
Sm@C82

0.2

0.8

0

0.6

1

5

10

50

100

500

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Sm Precipitate
Sm KOHSm Toluene
La Precipitate
La KOH
La Toluene

0.4

Fig. 3. The fraction yields of 140La and 153Sm in
dissolved precipitate through a Sephadex G25 asfunction time of reaction time.

References
1. K. Akiyama et al., J. Phys. Chem. A, 104, 7224
(2000).
2. J. Li et al., J. Chem. Soc. Chem. Commun., 1993,
1784 (1993).

0.2

0
1

5

10

50

100

500

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Fig.2. The activity ratios of 140La and 153Sm in threephases as function of reaction time.

ᡂᯝࡢබ⾲
Ꮫ⾡ㄅ
1.
K. Sueki and Y. Iwai, “Synthesis ofradio-metallofullerenols” J. Radioanal. Nucl.
Chem., 272 (2007) 505-509.
Ꮫ఍Ⓨ⾲
1. ⛅ᒣ࿴ᙪࠊྂᕝⱥ඾ࠊ㰻⸨㝧༤ࠊ℈㔝㐩⾜ࠊᮎᮌၨ௓ࠊ∦⏣ඖᕫࠊࣆࣞࢽࣝᅛᐃ┦ࢆ⏝࠸ࡓࣛࣥࢱࣀ࢖ࢻ㔠ᒓࣇ࣮ࣛࣞࣥࡢ +3/& ⁐㞳ᣲື࡟㛵ࡍࡿ◊✲➨  ᅇᨺᑕ໬Ꮫウㄽ఍ ᖺ ᭶ᮾி
2. ᮎᮌၨ௓ࠊ㛗ᓮⰾ⣖ࠊୖྖᬛ⩏ࠊ⛅ᒣ࿴ᙪࠊሯ
⏣࿴᫂ࠊὸ஭㞞ேࠊ㇏ᔱཌྐࠊỌ┠ㅍ୍㑻ࠊỈ

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JAEA-Review 2013-039

3.

⁐ᛶᨺᑕᛶྠ఩యෆໟࣇ࣮ࣛࣞࣥࡢྜᡂ➨ ᅇᨺᑕ໬Ꮫウㄽ఍ ᖺ  ᭶ᮾி
K. SUEKI, Y. Nagasaki, T. Kamitsukasa, K.
AKIYAMA, K. TSUKADA, M. ASAI, A.
TOYOSHIMA, Y. NAGAME, “S yn the s is of
w a ter- so luble en cap sul a t ed - r ad io is o top e
fu ller enes” APSO RC09 , D ec. 2009, N apa.

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JAEA-Review 2013-039

3-21
ᩥ໬㈈㕲㛵㐃㈨ᩱ࠾ࡼࡧ⎔ቃヨᩱ୰ࡢᚤ㔞ඖ⣲ࡢᣲື࡟㛵ࡍࡿ◊✲
Determination of trace elements in old iron and tea leaves as environmental standard candidate byneutron activation analysis
ᖹ஭᫛ྖࠊຍ⸨ᑗᙪࠊᒸ⏣ Ꮚ㸸Shoji HiraiࠊMsahiko KatoࠊYukiko Okada
ᮾி㒔ᕷ኱Ꮫ(ᪧ Ṋⶶᕤᴗ኱Ꮫ) ᕤᏛ㒊㸸Faculty of EngineeringࠊTokyo City University(Musashi Institute of Technology)࡛ከඖ⣲ࢆ㧗ឤᗘ࡛┿ᗘ㧗ࡃᐃ㔞࡛ࡁࡿᮏἲࡣࠊ᭱

㸯㸬ࡣࡌࡵ࡟ ⣙  ᖺ๓࡟ே㢮ࡀጞࡵ࡚㕲ࢆ౑⏝ࡋ࡚௨᮶㐺࡞᪉ἲ࡛࠶ࡿࠋ

Ọ㐲࡜⌧௦ࡲ࡛㕲ࡣᅜᐙᙧᡂࡢ♏࡜࡞ࡾࠊ౑⏝ࡉࢀᚑ᮶ࡢࢃࢀࢃࢀࡢ◊✲ᡂᯝ࡟ࡼࡿ࡜ࠊ㕲ᮦ࠶ࡿ࠸࡚࠸ࡿࠋ㕲㖔▼࠶ࡿ࠸ࡣ◁㕲ࢆཎᩱ࡜ࡋ࡚㕲సࡾࡢࡣ㕲ჾ୰ࡢࣄ⣲(As)࡜࢔ࣥࢳࣔࣥ(Sb)ࡢ⃰ᗘẚ࠿ࡽᢏ⾡ࡣࠊⓎ⚈ࢆす࢔ࢪ࢔ᆅ᪉࡛࠶ࡾࠊࣄࢵࢱ࢖ࢺᖇ

㕲ᮦ࠶ࡿ࠸ࡣ㕲ჾࢆ⏕⏘ࡋࡓ㕲ཎᩱࡢ⏘ᆅ᥎ᐃࢆྍ

ᅜࡢᇶ┙࡜ࡋ࡚㕲⏕⏘ᢏ⾡ࡣ☜ᅛ࡜ࡋࡓࡶࡢ࡜ࡋ࡚

⬟࡟ࡍࡿࡇ࡜ࡀ࡛ࡁࡓࠋࡲࡓࠊ㕲⏕⏘࡟㛵㐃ࡋ࡚᤼ᮾ࢔ࢪ࢔ࠊ༡࢔ࢪ࢔ࠊ࣮ࣚࣟࢵࣃ࡜⤒῭࡜ໃຊࡢᣑ

ฟࡉࢀࡿ㕲⁦࡟࠾࠸࡚ࡣࠊ㕲⁦࡟ྵ᭷ࡉࢀ࡚࠸ࡿࢳ

኱࡜࡜ࡶ࡟ୡ⏺୰࡟ᗈࡲࡗ࡚ࡁࡓࠋࢃࡀᅜ࡟࠾࠸࡚

ࢱࣥ(Ti)࡜ࣂࢼࢪ࣒࢘(V)ࡢ⃰ᗘẚ࠿ࡽ㕲⏕⏘࡟㛵ಀࡣࠊᘺ⏕ᮎᮇ 㹼 ୡ⣖㡭 ࡟ࡣ୰ᅜ࠶ࡿ࠸ࡣ㡑ᅜ࠿ࡍࡿ㕲ཎᩱࡢ⏘ᆅ᥎ᐃࢆྍ⬟࡟ࡋ࡚࠸ࡿࠋࡉࡽ࡟ࠊ

ࡽ㟷㖡ჾ࡜࡜ࡶ࡟㕲ჾࡶὶධࡋ࡚࠸ࡓࠋࡑࡢᚋࠊ

㑇㊧ࡢᛶ㉁ࠊࡍ࡞ࢃࡕࠊᙜ᫬᧯ᴗࡉࢀ࡚࠸ࡓ㕲సࡾୡ⣖࠿ࡽ  ୡ⣖࡟࠿ࡅ࡚㕲సࡾࡶࢃࡀᅜ⊂≉࡞ࡓࡓࡢࣉࣟࢭࢫࢆ㕲⁦ࡢᡂศ࠿ࡽ᥎ᐃࡍࡿࡇ࡜ࡶྍ⬟࡟ࡽ〇㕲ἲ࡟ࡼࡾ㕲సࡾࡀ⾜ࢃࢀ࡚ࡁࡓࠋ

ࡍࡿࡇ࡜ࡀ࡛ࡁࡿࠋ

⌧ᅾࠊᅵᆅࡢ㛤Ⓨࡸᘓ㐀≀ࡢಟ᚟࡟కࡗ࡚ྂ௦ࡶ

ࡑࢀࡺ࠼ࠊᮏ◊✲࡛ࡣࠊᵝࠎ࡞㑇㊧࠿ࡽฟᅵࡋࡓ

ྵࡵ࡚ྂ࠸㕲ࡀฟᅵࡋ࡚࠸ࡿࠋࡇࡢࡼ࠺࡞㕲ࡣࠊᩥ㕲ᮦ࠶ࡿ࠸ࡣ㕲ჾࢆ୰ᛶᏊᨺᑕ໬ศᯒࡋࠊ๓㏙ࡋࡓ໬㈈㈨ᩱ࡜ࡋ࡚㈗㔜࡞ࡶࡢ࡜ࡋ࡚ྲྀࡾୖࡆࡽࢀࠊྛ≉㉁ࢆゎ᫂ࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡋࡓࠋࡉࡽ࡟ࠊᩥ໬㈈ᆅࡢ༤≀㤋ࡸᇙⶶᩥ໬㈈ࢭࣥࢱ࣮➼࡟཰ⶶࡉࢀ࡚࠸

㕲㛵㐃㈨ᩱ࡜ࡣ␗࡞ࡿࡀࠊ୰ᛶᏊᨺᑕ໬ศᯒࡢ≉ᚩࡿࠋࡋ࠿ࡋࠊ㕲ࡢ⏕⏘ᢏ⾡ࠊ㕲ࡢὶ㏻㐣⛬ࠊ㕲సࡾࡢ୍ࡘ࡛࠶ࡿ┿ᗘࡢ㧗ࡉࢆ⏕࠿ࡋࡓ⎔ቃᶆ‽≀㉁ೃ

ࡢࡓࡵࡢ㕲ཎᩱࡢ✀㢮࣭⏘ᆅࡸ㕲ࡢᮦ㉁➼ࡢ▱ぢࢆ⿵࡜࡞ࡿヨᩱࡢ್௜ࡅࡢඹྠศᯒ࡟ཧ⏬ࡋࡓࠋྛ✀ᚓࡿࡓࡵ࡟ࡣࠊ཰ⶶࡔࡅ࡛ࡣఱࡶࢃ࠿ࡽࡎࠊ⮬↛⛉ศᯒἲ࡟ࡼࡿ್௜ࡅࡀ⤊஢ࡋࡓᚋ࡟ࡣࠊㄆド್࡜ࡋᏛⓗ࡞ㄪᰝ࡜ᩥ໬㈈࣭ᕤᏛⓗ࡞ㄪᰝ࡛ࡣࡌࡵ࡚ᙜ᫬

࡚බ⾲ࡉࢀࠊᮏᶆ‽≀㉁ࢆ฼⏝ࡋ࡚ከࡃࡢ⎔ቃヨᩱసࡽࢀࡓ㕲ࡢጼࡢ୍㠃ࢆᤊ࠼ࡿࡇ࡜ࡀ࡛ࡁࡿࠋ

ࡢศᯒ್ࡢಙ㢗ᛶ☜ಖࡢ୍ຓ࡜ࡋ࡚㈉⊩ࡍࡿࡇ࡜ࡀ

ᮏ◊✲ࡣࡇࡢࡼ࠺࡞⫼ᬒࡢୗࠊ㕲ᮦ࣭㕲ჾ࡟ྵ᭷ᮇᚅࡉࢀ࡚࠸ࡿࠋ

ࡍࡿᚤ㔞ඖ⣲ࡢ╔┠ࡋࠊ㕲ࡢᮦ㉁ࠊ㕲ཎᩱࡢ᥎ᐃ࠾
ࡼࡧ㕲ཎᩱࡢ⏘ᆅ᥎ᐃࢆ⾜࠺࡞࠺ࡇ࡜ࢆ┠ⓗ࡜ࡋࠊ㸰㸬᚟ ඖࡓࡓࡽ࡟ࡼࡿ⏕⏘ࡉࢀࡿ㕲࠾ࡼࡧ㕲⁦୰ࡢᚤ㔞ඖ⣲ࡢᣲື

୰ᛶᏊᨺᑕ໬ศᯒࢆ⾜ࡗࡓࠋࡲࡓࠊ୰ᛶᏊᨺᑕ໬ศ
ᯒἲࡢ㑅ᢥࡢ⌮⏤ࡣࠊᩥ໬㈈㈨ᩱ࡛࠶ࡿ㕲ᮦ࣭㕲ჾ  ᖺ 11 ᭶ 5 ᪥㹼6 ᪥࡟⚟ᓥ┴ᩥ໬㈈ࢭࣥࢱ࣮

ࡣ㈗㔜࡞ࡓࡵከࡃࡢヨᩱࢆศᯒ࡟౪ࡍࡿࡇ࡜ࡀ࡛ࡁⓑἙ㤋ࠗࡲ࡯ࢁࢇ࠘࡟࠾࠸࡚ࠊ㺀㕲సࡾ㺁࢖࣋ࣥࢺࡀ

࡞࠸ࡇ࡜࡜ྜࢃࡏ࡚ࠊ㕲ࡢ໬Ꮫⓗᛶ㉁࡛᫬௦࡜࡜ࡶ

⾜ࢃࢀࡓࠋࡇࡇ࡛ࡣࠊ◁㕲ࢆཎᩱ࡜ࡋ࡚ᖹᏳ᫬௦ࡢ

࡟㗵ࡧ࡚ᮙࡕ࡚࡞ࡃ࡞ࡿࡇ࡜ࡀከ࠸ࡢ࡛ࠊከ㔞ࡢヨ⅔ᙧࡢ኱ࡁࡉࢆ᚟ඖࡋࡓࡓࡓࡽ⅔ࡀ᧯ᴗࡉࢀࠊ㕲సᩱࢆᚓࡿࡇ࡜ࡀᅔ㞴࡞ࡇ࡜ࡀᣲࡆࡽࢀࠊᑡ㔞ࡢヨᩱࡾࡀ⾜ࢃࢀࡓࠋ

㸦◊✲᪋タࠊ⿦⨨ࠊ◊✲ศ㔝㸧
㸸JRR-4 Ẽ㏦⟶㸦Pn㸧 T-ࣃ࢖ࣉࠊȚ⥺Ἴ㧗ศᯒჾࢩࢫࢸ࣒ࠊᩥ໬㈈㕲㛵㐃
ヨᩱᨺᑕ໬ศᯒࠊ⎔ቃᶆ‽≀㉁ೃ⿵ヨᩱᨺᑕ໬ศᯒ

- 403 -

㻝㻢㻞

JAEA-Review 2013-039

 ᮏ◊✲࡛ࡣࠊࡇࡢ㕲〇㘐㐣⛬࡟࠾࠸࡚⏕⏘ࡉࢀࡓ୰ᛶᏊ↷ᑕࡢ᮲௳ࡣࠊ᪥ᮏཎᏊຊ◊✲㛤Ⓨᶵᵓࡢ㕲ሢཬࡧࢫࣛࢢ㸦㕲⁦㸧୰ࡢྵ᭷ඖ⣲⃰ᗘ࠿ࡽ〇㘐

JRR-4 ཎᏊ⅔(⇕ฟຊ 100kW)ࢆ฼⏝ࡋࡓࠋ୰ᛶᏊ↷㐣⛬࡟ࡼࡾ࡝ࡢࡼ࠺࡞ඖ⣲ࡀ࡝ࡢࡼ࠺࡞ᣲືࢆࡍࡿ

ᑕ᮲௳࠾ࡼࡧȚ⥺ᐃ᮲௳ࢆ⾲ 1 ࡟♧ࡍࠋ࡞࠾ࠊMn࠿ࢆホ౯ࡍࡿࡇ࡜ࢆ┠ⓗ࡜ࡋ࡚࠸ࡿࠋ

ࡢᐃ㔞࡛ࡣࠊ )H Q㹮 0Q཯ᛂ࡟ࡼࡾ 0Q ࡀ ศᯒヨᩱ⏕ᡂࡍࡿࡢ࡛ࠊ㧗⣧ᗘ㕲㸦0Q ᴟᚤ㔞㸧ࢆ⏝࠸࡚ )H ศᯒヨᩱࡣࠊᡭືࢲ࢖ࣖࣔࣥࢻ࢝ࢵࢱ࣮ࢆ౑⏝ࡋ࠿ࡽࡢᐤ୚㸦0QȣJ)HJ㸧ࢆィ⟬ࡋࠊ⿵ṇࢆ࡚㕲ሢࡢ㔠ᒓ㒊ࢆษ๐ࡋࡓࠋ◁㕲ཬࡧࢫࣛࢢヨᩱࡣ⾜ࡗࡓࠋࡲࡓࠊ&U ࡢᐃ㔞࡟࠾࠸࡚ࡣࠊ)H QȘ ⣙ᩘ㹥ࡢヨᩱࢆ࣓ࣀ࢘〇ங㖊࡟ࡼࡾ⢊○㸦100ȣm௨ୗ㸧
࣭ᆒ㉁໬ࡋࡓࡶࡢࢆ᥇ྲྀࡋࡓࠋ࠸ࡎࢀࡢヨᩱࡶᴟᚤ㔞㸧ࢆ⏝࠸࡚ )H ࠿ࡽࡢᐤ୚㸦&UȣJ)HJ㸧⣙ 50mg ࢆᨺᑕ໬ศᯒ⏝ࡢヨᩱ࡜ࡋࡓࠋ

ࢆィ⟬ࡋࠊ⿵ṇࢆ⾜ࡗࡓࠋ&U཯ᛂ࡟ࡼࡾ &U ࡀ⏕ᡂࡍࡿࡢ࡛ࠊ㧗⣧ᗘ㕲㸦&U ศᯒ᮲௳
⾲ 1 ୰ᛶᏊ↷ᑕ᮲௳࠾ࡼࡧȚ⥺ ᐃ᮲௳⇕୰ᛶᏊ᮰ᐦᗘ
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ࢀࡓࢫࣛࢢ࡛ࡣ⣙  ࡛࠶ࡗࡓࠋࡇࡢ࡜ࡁࡢ
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㻡㻟㻜㻝㻜㻜㻜㻜㻜㻜 㻖㻥㻜㻤 㻖㻨 㻝㻝㻣 㻖㻨 㻝㻝㻜㻨 㻟㻥㻚㻤 㻖㻢㻣㻚㻤 㻖
㻟㻡㻚㻤 㻖㻨 㻜㻚㻤㻟 㻖㻨 㻢㻤㻚㻣 㻖㻞㻝㻚㻝 㻖㻨 㻜㻚㻟㻝
㻝㻚㻥㻥 㻖㻨㻝㻟㻨 㻜㻚㻢㻥㻞 㻖㻨 㻝㻝㻟 㻖㻜㻚㻤㻤 㻖㻨 㻡㻚㻤㻝 㻖㻜㻚㻞㻡 㻖㻨 㻜㻚㻤㻤㻨 㻜㻚㻟㻞 㻖㻨 㻜㻚㻜㻥 㻖㻨 㻜㻚㻜㻥 㻖㻨 㻜㻚㻢㻠 㻖㻨 㻜㻚㻜㻜㻢㻣 㻖㻨 㻜㻚㻡㻜 㻖㻨 㻜㻚㻤㻡 㻖

㕲ሢ㻠
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㻞㻚㻝㻣
㻨㻝㻚㻠㻞

㻔㼜㼜㼙㻕
㕲ሢ䠄༺䛧䠅
䝇䝷䜾䠐
㘫෬⁦
㻡㻝㻚㻥
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㻨
㻜㻚㻥㻜
㻖
㻨㻜㻚㻣㻟
㻨㻞㻚㻠㻜
㻨㻜㻚㻜㻜㻟㻢㻨 㻜㻚㻜㻜㻢㻟 㻖 㻨㻜㻚㻜㻜㻢㻝
㻨
㻜㻚㻠㻠
㻖
㻠㻚㻤㻝
㻝㻜㻚㻤
㻖
㻨
㻜㻚㻢㻣
㻨㻝㻚㻠㻝
㻨㻞㻚㻜㻥
㻨䠖᳨ฟୗ㝈್௨ୗ䛾್䠆㻲㼑䜢㻝㻜㻜㻑䛸䛧䛶⿵ṇ䛧䛯್

3-21- 404 -

㻝㻢㻟

JAEA-Review 2013-039

㗵ࡧ࡚࠸ࡿ࠿⁦㒊ࡢヨᩱࡣࠊ)H ⃰ᗘࡀ 㸣௨ୗ㸱㸬బ㈡⸬཯ᑕ⅔㊧࠿ࡽฟᅵࡋࡓ㕲㛵㐃㈨ᩱ
Ụᡞᖥᮎᮇࡢ჆Ọ  ᖺ  ᖺࠊబ㈡⸬ ⌧ బ㈡࡜࡞ࡿࡀࠊ೺඲࡞㕲㔠ᒓ㒊ࢆṧࡋ࡚࠸ࡿ࡜ࡇࢁࡣ┴ ࡢ⠏ᆅ࡟ࢃࡀᅜ᭱ึࡢ཯ᑕ⅔ࡀᘓタࡉࢀࠊḟ࠸࡛㸣㏆ࡃࡢ್࡟࡞ࡿࠋࡑࢀࡺ࠼ࠊ)H ⃰ᗘ࠿ࡽ㗵ࡢ჆Ọ  ᖺ  ᖺ ࡟ከᕸ᪋࡟ࡶᘓタࡉࢀࡓࠋ཯ᑕ⅔

㐍⾜ᗘྜ࠸ࡸ⁦ࡢΰධ๭ྜࢆ᥎

࡟࠾࠸࡚ࡣࠊ኱◙ࡘࡃࡾ࡟㕲ࡀ⁐ゎࡉࢀࡿࡀࠊࡑࡢ

ࡢᗘྜ࠸ࡣࠊ&O ⃰ᗘ࠿ࡽࡶ᥎ ࡛ࡁࠊࡇࢀࡽࡢヨᩱ㕲ཎᩱࡀࢃࡀᅜࡢࡶࡢ࠿ࠊእᅜ࠿ࡽ㍺ධࡉࢀࡓࡶࡢ

ࡣ⁦ࡶྵࡲࢀࡿࡀࠊ)H ࡀ㗵ࡧࡓࡶࡢ࡛࠶ࡿࡇ࡜ࡀࢃ

࠿ࠊ࠶ࡿ࠸ࡣ◁㕲ཎᩱ࡜ࡋࡓࡶࡢ࠿ࠊ㕲㖔▼ཎᩱ࡜࠿ࡿࠋ࡛ࡁࡿࠋࡲࡓࠊ㗵ࡋࡓࡶࡢ࠿ᮍࡔゎ᫂ࡉࢀ࡚࠸࡞࠸ࡇ࡜ࡀከ࠸ࠋᮏ◊ࡲࡓࠊ◁㕲ཎᩱࡢᣦᶆ࡜࡞ࡿ 7L ࡸ 9 ⃰ᗘࡀ᳨ฟࡉ

✲࡛ࡣࡇࢀࡽࡢࡇ࡜ࢆゎ᫂ࡍࡿࡓࡵࠊ୰ᛶᏊᨺᑕ໬

ࢀ࡞࠸࠶ࡿ࠸ࡣᑠࡉ࠸ࡇ࡜࡜ࠊ㕲㖔▼࡟ẚ㍑ⓗ≉ᚩศᯒࢆ⾜ࡗࡓࠋ

࡞ &X ⃰ᗘࡀ㧗࠸ࡇ࡜࠿ࡽࡇࢀࡽࡢ㕲ཎᩱ≀㉁ࡣࠊ㕲ศᯒヨᩱࡢࡓࡵࡢ๓ฎ⌮ࡸ୰ᛶᏊ↷ᑕ᮲௳࠾ࡼࡧ

㖔▼࡛࠶ࡿࡇ࡜ࡀ᥎ᐹ࡛ࡁࡓࠋ
ศᯒࡋࡓヨᩱࡢ㕲ཎᩱࡢྠ୍ᛶࢆࡳࡿࡓࡵ࡟ࠊȚ⥺ ᐃ᮲௳ࡣࠊ ࠾ࡼࡧ  ࡟♧ࡋࡓ᮲௳࡜࡯
ࡰྠᵝ࡞ࡢ࡛┬␎ࡍࡿࠋ

$V6E ⃰ᗘẚࢆ⾲  ࡟♧ࡋࡓࠋ⾲࠿ࡽ᫂ࡽ࠿࡞ࡼ࠺

 ⤖ᯝཬࡧ⪃ᐹ࡟ 61 ࡜ 61 ࡢྠ୍ᛶࢆ㝖ࡅࡤࠊ඲࡚␗࡞ࡗ࡚࠸

ศᯒࡋࡓヨᩱࡣࠊ㕲⁦㸦61㸧ࠊ㕲Წ∦㸦61㸧ࠊ኱◙㕲㗵∦㸦61ࠊ61㸧ࠊ㕲⁦㸦ᑠࡉ࡞㕲⢏ࢆྵࡓࠋ࡞࠾ࠊྠ୍ヨᩱ࡛࠶ࡿ 61P ࡜ 61㹱ࡢ್ࡣࠊᙜ↛࡞ࡀࡽྠ୍ࡢ್࡟࡞ࡗ࡚࠸ࡿࠋ

ࡴ㸧㸦61㹫ࠊ61㹱㸧 Ⅼ࡛࠶ࡿࠋ61P ࡜ 61Vᨺᑕ໬ศᯒࢆ⾜ࢃ࡞࠿ࡗࡓࡀࠊ኱ࡁ࡞ྠ୍㑇≀ヨ࡜ࡢ㐪࠸ࡣࠊྠ୍㑇≀ヨᩱࡢ㔠ᒓ㒊࡜⁦㒊࠶ࡿ࠸ࡣᩱࡢู࡞⟠ᡤࡢヨᩱ 61 ࡢ㕲㔠ᒓ㒊ࡀṧᏑࡍࡿ㗵㒊࡛࠶ࡿࠋࡇࢀࡽࢆศᯒࡋࡓ⤖ᯝࢆ⾲  ࡟♧ࡍࠋ61P ࡢ㔠ᒓ⤌⧊ࢆ (30$ ࡛ほᐹࡋࡓᅗࢆᅗ  ࡟♧ࡍࠋ඲యࡀ )H ࡛࠶ࡿࡇ࡜ࡀࢃ࠿ࡿࡀࠊᅗ୰ኸ㒊࡟ࡣ⾲ 3 బ㈡⸬཯ᑕ⅔㊧࠿ࡽฟᅵࡋࡓ㕲㑇≀

6 ࡀᏑᅾࡋ࡚࠸ࡿࡇ࡜ࡀࢃ࠿ࡿࠋᜍࡽࡃ &X6 ࡢᙧ࡛࠾ࡼࡧ኱◙㕲㗵ࡢศᯒ⤖ᯝ
Na
Mg
Al
Cl
K
Ca
Sc
Ti
V
Cr
Mn
Fe
Ni
Co
Cu
Ga
As
Br
Sb
Cs
Hf
Ce
Yb
La
Sm
W
Th
U
As/Sb

䠄䃛㼓㻛㼓㻌䠖㻌㼜㼜㼙䠅
SN-14m SN-14s
9.3
8900<5600 <12000
150
51000
640
<270
15000
䠉
䠉
<810
<1200
6.6
0.043
6.6
0.04
䠉
䠉
䠉
<79
<110
<240
<350
570
4400
12
49
64
150
1600
530
67
69
78
120
570
180
27
120
1600
2900
3900
7200
830000 1000000 700000 700000 990000
92000
360
680
䠉
150
310
䠉
220
200
110
100
240
15
230
610
260
110
590
<340
4.8
52
15
53
75
26
36
310
22
410
14
5.2
2.0
6.6
3.7
1.1
䠉
2.0
3.4
17
3.6
12
0.44
1.9
䠉
䠉
䠉
䠉
䠉
Ɇ
0.71
0.26
3.9
䠉
䠉
32
䠉
䠉
䠉
䠉
䠉
1.5
䠉
䠉
䠉
䠉
䠉
0.50
0.36
12
0.34
䠉
䠉
2.5
0.71
0.15
7.8
9.2
110
2.3
4.9
2.0
4.6
䠉
䠉
䠉
䠉
䠉
1.3
0.43
0.50
0.49
0.42
0.72
13
11
18
6
34
32
䠉䠖᳨ฟ䛥䜜䛪
䠘䠖ᐃ㔞ୗ㝈್௨ୗ䛾್
SN-3
110
<630
430
420
270
<990

SN-5
5.2
<1200
15
2200

SN-10
840
<1600
18
2200
360
<770

SN-11
190
<2300
72
1800
170
1100

Ꮡᅾࡋ࡚࠸ࡿࡶࡢ࡜ᛮࢃࢀࠊ⾲  ࡟࠾ࡅࡿ㧗⃰ᗘ࡞
&X ࡢᏑᅾࢆ⿬௜ࡅࡿࡶࡢ࡜᥎ᐹ࡛ࡁࠊ㕲ཎᩱ୰࡟ࡇ
ࡢࡼ࠺࡞໬ྜ≀ࡀᏑᅾࡋ࡚࠸ࡿࡇ࡜ࢆ♧၀ࡍࡿࠋࡲ
ࡓࠊ& ⃰ᗘࡀ⥺≧࡟㧗⃰ᗘ࡛ࡳࡽࢀࡿࡢࡣࠊ)H ୰࡟ࢭ࣓ࣥࢱ࢖ࢺ㸦)H&㸧ࡀከࡃᏑᅾࡋࠊ㕲⮬యࡀ㗪㕲ࡢ≧ែ࡟࠶ࡿࡇ࡜ࢆ♧ࡍࡶࡢ࡛࠶ࡿࠋ

- 405 -

  㕲⁦୰࡟ྵ᭷ࡍࡿ )H 㔠ᒓ㒊ࡢ (30$ ゎᯒീ
ᅗ


3-21



㻝㻢㻠

JAEA-Review 2013-039

㸲㸬㇏ᓥ༊ᕢ㬞㑇㊧࠿ࡽฟᅵࡋࡓ㕲㔥⾲  ᕢ㬞㑇㊧࠿ࡽฟᅵࡋࡓ㕲㔥ࡢศᯒ⤖ᯝ㇏ᓥ༊ᕢ㬞㑇㊧࣭ࣁ࣮ࣔࢽ࣮ࣁ࢖ࢶᆅ༊ࡢ㑇ᵓࡣࠊㄪᰝ㠃✚  ੍࡛ࠊ ᖺ㸲᭶㹼㸴᭶࡟ㄪᰝࡉࢀ
ࡓ㑇ᵓ࡛࠶ࡿࠋ୰ᒣ㐨ࡢ⾤㐨ἢ࠸ࡢ⏫ሙ࡛㘫෬ᒇ࡛࠶ࡗࡓ࡜ᛮࢃࢀࡿ㑇ᵓ࡛࠶ࡾࠊỤᡞ᫬௦ࡢᖥᮎ࠿ࡽ
᫂἞࡟࠿ࡅ࡚ࡢ᫬ᮇࡢࡶࡢ࡛࠶ࡿࠋᮏ㑇ᵓࡢ࠺ࡕ ྕ㑇ᵓ࡛ࡣࠊ࡯ࡰྠࡌ㕲㔥ࡀከ㔞࡟ฟᅵࡋࠊ㔥ࡢࣜࢧ࢖ࢡࣝࡀ⾜ࢃࢀ࡚࠸ࡓࡇ࡜ࡀ᥎ᐃ࡛ࡁࡿࠋᮏ◊✲࡛ࡣࠊࡇࢀࡽࡢ㔥ࡀ࡝ࡢࡼ࠺࡞≉㉁ࢆᣢࡗ࡚࠸ࡿ࠿
ࢆㄪᰝࡍࡿࡓࡵࠊ୰ᛶᏊᨺᑕ໬ศᯒࢆ⾜ࡗࡓࠋศᯒヨᩱࡢࡓࡵࡢ๓ฎ⌮ࡸ୰ᛶᏊ↷ᑕ᮲௳࠾ࡼࡧȚ⥺ ᐃ᮲௳ࡣࠊ ࠾ࡼࡧ  ࡟♧ࡋࡓ᮲௳࡜࡯
ࡰྠᵝ࡞ࡢ࡛┬␎ࡍࡿࠋ
 ⤖ᯝཬࡧ⪃ᐹศᯒࡋࡓ㕲㔥ࡣࠊ㛗ࡉ 㹼FPࠊ㔜ࡉ 㹼J ࡢᅄゅ࠸ⓙᢡ㔥࡛ࠊ⾲㠃ࡣ㗵ࡧ࡚࠸ࡿࡀෆ㒊ࡣ೺඲࡞㔠ᒓ㒊ࡀṧࡗ࡚࠸ࡿࠋⅣ⣲⃰ᗘࡀ 㹼㸣࡜㌾㕲
࡟ᒓࡍࡿࡶࡢ࠿ࡽࠊ㹼㸣ࡢపⅣ⣲㗰࡟ᒓࡍࡿࡶࡢ࡛࠶ࡿࠋ⾲  ࡟ࡣ  ᮏࡢ㕲㔥ࢆ୰ᛶᏊᨺᑕ໬ศᯒࡋࡓ⤖ᯝࢆ♧ࡍࠋ)H ⃰ᗘࡀ࡯ࡰ 㸣࡛࠶ࡿࡇ࡜࠿ࡽࡶ೺඲
࡞㔠ᒓ㒊ࡀṧᏑࡋ࡚࠸ࡿࡇ࡜ࡀࢃ࠿ࡿࠋᮏヨᩱ୰࡟ᐃ㔞 ್(ppm )
SG-1
SG-2
SG-3
SG-4
SG-5
ᕢ 㬞㑇㊧ ᕢ 㬞㑇 ㊧ ᕢ 㬞㑇 ㊧ ᕢ㬞㑇 ㊧ ᕢ 㬞㑇㊧
ඖ⣲
㕲㔥
㕲㔥
㕲㔥
㕲㔥
㕲㔥
Na
100
34
53
26
140
Mg
<360
<320
<290
<310
<290
Al
120
120
240
150
130
Cl
260
<13
<28
25
120
K
200
40
44
<36
57
Ca
<160
<200
<200
<200
530
Sc
0.12
0.41
0.36
0.48
0.45
Ti
<70
<66
<57
<68
<58
V
33
53
32
27
37
Cr
43
42
35
33
41
Mn
270
570
380
450
570
Fe
1030000 980000 1000000 970000 960000
Co
78
89
110
110
64
Ni
190
240
240
180
160
Zn
<25
<18
15
<21
<20
Ga
25
20
20
17
As
450
130
470
130
120
Se
<1.7
<2.5
<2.1
<2.3
Br
1.1
0.61
<0.60
<0.50
<0.57
Rb
17
<13
43
<16
<15
Zr
<230
<290
<270
<260
<210
Ag
23
13
45
<13
41
Sb
27
220
63
220
40
Te
<61
<62
<100
<78
<92
I
<3.1
<2.8
<3.4
<2.8
<3.6
Cs
<0.38
15
130
39
130
Ba
<67
<91
<81
<83
<93
La
0.25
0.28
0.35
0.17
0.13
Ce
<2.1
<2.5
<2.5
<2.5
<2.4
Sm
<0.081<0.049<0.097<0.058<0.089
Tb
<0.22
<0.27
<0.26
<0.24
<0.42
Yb
<0.21
<0.14
<0.23
<0.18
<0.21
Lu
<0.025<0..038<0.031<0.035<0.041
Hf
<0.47
<0.31
<0.42
<0.37
<0.38
Ta
<0.33
<0.52
<0.38
<0.41
Au
0.008
0.022
0.13
<0.0042
0.22
Hg
<0.42
Th
<0.30
<0.20
<0.31
<0.25
<0.28
U
<1.0
As/Sb
3.2
4.3
2.1
2.1
2.1

SG-6
ᕢ 㬞㑇㊧
㕲㔥
95
350
390
210
350
<420
0.36
<29
10
69
40
1010000
150
470
<20
46
0.96
18
<170
7.1
2.7
<43
<1.3
<0.68
<72
0.18
<1.8
<0.024<0.33<0.15<0.030<0.36<0.0040
<0.27
<0.22
<0.65
16.6

ࡣ㕲୰࡟⃰㞟ࡋࡸࡍ࠸ &Rࠊ1Lࠊ$Vࠊ6E ࡀ㧗⃰ᗘ࡛Ꮡᅾࡋ࡚࠸ࡓࠋ≉࡟ࠊ㕲ཎᩱࡢᣦᶆ࡜࡞ࡿ $V6E ⃰ᗘẚࡣࠊ6* ࢆ㝖࠸࡚࡯ࡰ 㹼 ࡢ್࡛࠶ࡾࠊࡇࢀࡽ
ࡢ㕲㔥ࡣྠ୍ࡢ㕲ཎᩱ࡟ࡼࡾసࡽࢀࡓࡶࡢ࡛࠶ࡿࡇ
࡜ࡀ᥎ᐹ࡛ࡁࡿࠋ࡞࠾ࠊඖ⣲⃰ᗘࡔࡅࡢ᝟ሗ࡛ࡣࠊ
㕲ཎᩱࡢ✀㢮ࢆ≉ᐃ࡛ࡁ࡞࠸ࡀࠊ(30$ ࡢゎᯒീ࡛☜ㄆࡍࡿ࡜ 3 ࡀ㧗⃰ᗘ᳨࡛ฟࡉࢀ࡚࠸ࡿࡇ࡜࠿ࡽ㕲㖔ࡋࠊ⯪㏻ᒣ࡛㙾㕲㖔ࡀ⏘ࡍࡿ࡜࡞ࡿ࡜ࠊࡇࡢ㕲㖔▼ࢆ฼⏝ࡋ࡚࡝ࡢࡼ࠺࡞㕲ࡀ࡛ࡁࡿ࠿ࡣࠊ㠀ᖖ࡟⯆࿡࠶ࡿࡇ࡜࡛࠶ࡿࠋᮏ◊✲࡛ࡣࠊࡇࡢᆅ᪉࡛⏘ࡋࡓ㙾㕲㖔ࢆ฼⏝ࡋࡓᶍᨃࡓࡓࡽᐇ㦂࡜ࠊ௚ᆅᇦࡢရ㉁ࡢ
ࡼ࠸㙾㕲㖔ࢆ⏝࠸࡚ᶍᨃࡓࡓࡽᐇ㦂ࢆ⾜ࡗࡓࠋࡇࡢ
ᐇ㦂ࢆ㏻ࡋ࡚ࡢྛඖ⣲ࡀ࡝ࡢࡼ࠺࡞ඹྠࢆࡍࡿ࠿ࢆ
ㄪᰝࡢ┠ⓗ࡜ࡋࡓࠋ

▼⏤᮶࡛࠶ࡿࡇ࡜ࡀ᥎ᐃ࡛ࡁࡓࠋ

ศᯒヨᩱࡢࡓࡵࡢ๓ฎ⌮ࡸ୰ᛶᏊ↷ᑕ᮲௳࠾ࡼࡧ

㸳㸬㙾㕲㖔ࢆཎᩱ࡜ࡋࡓᶍᨃࡓࡓࡽ〇㕲࡟ࡼࡿྛඖȚ⥺ ᐃ᮲௳ࡣࠊ ࠾ࡼࡧ  ࡟♧ࡋࡓ᮲௳࡜࡯
ࡰྠᵝ࡞ࡢ࡛┬␎ࡍࡿࠋ

⣲ࡢᣲື㫽ྲྀ┴᪥༡⏫࡜ᓥ᰿┴ዟฟ㞼⏫ࡢ┴ቃ࡟࠶ࡿ⯪㏻ ⤖ᯝཬࡧ⪃ᐹྛ✀㙾㕲㖔ࢆศᯒࡋࡓ⤖ᯝࢆ⾲  ࡟♧ࡍࠋ⾲୰ࡢᒣࡣࠊ㺀ඵᒱ኱⺬㺁ࡢ⚄ヰ࡟࡞ࡗࡓ⯙ྎ࡛ࠊ⯪㏻ᒣ࠿
ࡽࡣ㉥㕲㖔ࡢ୍✀࡛࠶ࡿ㙾㕲㖔ࡀ⏘ࡍࡿࡇ࡜ࡀ▱ࡽࢀ࡚࠸ࡿࠋྂ௦࡟࠸࡚㫽ྲྀ┴ࡸᓥ᰿┴࡛ᩘከࡃࡢࡓ
ࡓࡽ〇㕲ࡀ⾜ࢃࢀ࡚ࡁࡓࡀࠊ୍⯡࡟ࡣࡇࡢᆅ᪉࡛⏘ࡍࡿ◁㕲ࡀ฼⏝ࡉࢀ࡚㕲సࡾࡀ⾜ࢃࢀ࡚ࡁࡓࠋࡋ࠿

)H ⃰ᗘࢆࡳࡿ࡜ࠊ㹼㸣࡜ᖜᗈࡃࡤࡽࡘ࠸࡚࠸ࡿࠋ
)H ⃰ᗘࡀ㧗ࡅࢀࡤࡑࢀࡔࡅ㙾㕲㖔ࡢရ఩ࡀ㧗ࡃࠊ㏫࡟పࡅࢀࡤရࡣᝏࡃ࡞ࡿࠋࡍ࡞ࢃࡕࠊရ఩ࡀᝏ࠸࡜
࠸࠺ࡇ࡜ࡣࠊࡑࢀࡔࡅ⬦▼ᡂศࡀከ࠸࡜࠸࠺ࡇ࡜࡟

- 406 -

3-21
㻝㻢㻡

JAEA-Review 2013-039

࡞ࡾࠊࡑࢀࡔࡅ୙⣧≀ඖ⣲ࡀከ࠸࡜࠸࠺ࡇ࡜࡟࡞ࡿࠋ

࡛ࡁ࡞࠿ࡗࡓࠋࡋ࠿ࡋࠊ㕲ሢ࡜㕲⁦ ࢫࣛࢢ ࡜ࡢ㛫ࡇࡢࡼ࠺࡞ほⅬ࠿ࡽࡍࡿ࡜ࠊ⬦▼ᡂศࡢከࡃࡣ㛗▼࡛ࠊ≉ᐃࡢඖ⣲ࡀ࡝ࡕࡽ࠿࡟⃰㞟ࡍࡿഴྥࢆࡳࡿࡇ

㢮ࡸ▼ⱥ࡜࡞ࡿࠋ㛗▼ࡣ .2 ࡀከࡃྵ᭷ࡉࢀࠊ▼ⱥ࡜ࡀ࡛ࡁࡓࠋ⣽࠿࠸ᩘ್ࡣࡇࡇ࡛ࡣ┬␎ࡍࡿࠋ


ࡣ 6L2 ࡀᡂศ࡜࡞ࡿࡀࠊᨺᑕ໬ศᯒ࡛ࡣࠊ. ࡋ࠿ᐃ㔞࡛ࡁ࡞࠸ࡀࠊ)H ⃰ᗘ࡜㏫┦㛵ࡀࡳࡽࢀࡿࠋࡲࡓࠊ㸴㸬 ⯙ᓮ㑇㊧ฟᅵࡢ㕲ᮦࡢᮦ㉁

┦㛵ᛶࡣᚲࡎࡋࡶ࡞࠸ࡀࠊ7Lࠊ0Qࠊ&Rࠊ$V ࡢ㛫࡟ࡶ⯙ᓮ㑇㊧ࡣࠊ⚟஭┴ᩔ㈡ᕷ࡟఩⨨ࡋࠊᘺ⏕᫬௦࠿኱ࡁ࡞⃰ᗘࡢࡤࡽࡘࡁࡀࡳ࠼࡚ࡃࡿࠋ≉࡟ࠊྠ୍ᆅ

ࡽྂቡ᫬௦๓ᮇ࡟࠿ࡅ࡚ከࡃࡢఫᒃ㊧ࡸྂቡ࠿ࡽ࡞

ᇦࡢ㙾㕲㖔࡜࡞ࡿ࡜ $V6E ⃰ᗘẚࡀ⯆࿡῝࠸ࠋ Ⅼࡿ㑇㊧࡛࠶ࡿࠋ௒ᅇࠊࡇࡢ࠺ࡕࡢ  ྕྂቡ࡜  ྕྂࡢヨᩱ࡟ࡘ࠸࡚ࡣࠊ$V ࠶ࡿ࠸ࡣ 6E ࡀᐃ㔞ୗ㝈್௨ቡࡢ୰࠿ࡽ୙᫂ᯈ≧㕲〇ရࡀฟᅵࡋࡓࠋᅗ  ࡣ  ྕୗࡢ್࡛࠶ࡗࡓࡢ࡛ẚ㍑ࢆࡍࡿࡇ࡜ࡀ࡛ࡁ࡞࠸ࡀࠊ

ྂቡ࠿ࡽฟᅵࡋࡓ୙᫂ᯈ≧㕲〇ရ㸦70㸧㸦㛗ࡉ.1$ ࡢヨᩱࢆ㝖࠸࡚࡯ࡰྠ୍ࡢ್࡛࠶ࡗࡓࠋ

FPᖜ 㹼FPཌࡉ 㹼FPࠊ㔜ࡉ

.1$ ࡢヨᩱࡣ㇂ᕝࡢ୰࡛᥇ྲྀࡋࡓヨᩱ࡛࠶ࡿࡇ

J㸧ࡢᴫほ࡛࠶ࡿࠋศᯒࡣࠊᅗ୰ྑୗ࡟࠶ࡿࡼ࠺

࡜࠿ࡽࠊ௚ࡢᆅᇦ࠿ࡽᕝࡢὶࢀ࡟ࡼࡗ࡚㐠ࡤࢀࡓࡶ࡞࡜ࡇࢁ࠿ࡽヨᩱࢆษࡾฟࡋࡓࠋ ྕྂቡ࠿ࡽࡶྠ

ࡢ࡜᥎ᐃ࡛ࡁࠊ್ࡀ␗࡞ࡗࡓࡶࡢ࡜ᛮࢃࢀࡿࠋ

ᵝ࡞ヨᩱ 70P ࢆษࡾฟࡋࡓࠋ70P ࡣ᫂ࡽ࠿࡟㔠ᶍᨃࡓࡓࡽᐇ㦂࡛ࡣࡇࢀࡽ㙾㕲㖔ࢆΰࡐ࡚౑⏝ࡋᒓ㒊ࡀぢ࠼ࡓࡀࠊ70 ࡣ඲࡚㗵ࡧ࡚࠸ࡓࠋ

ࡓࡢ࡛ࠊࡓࡓࡽᐇ㦂࡟ࡼࡾ⏕⏘ࡉࢀࡓ㕲ሢࡢྛඖ⣲ศᯒヨᩱࡢࡓࡵࡢ๓ฎ⌮ࡸ୰ᛶᏊ↷ᑕ᮲௳࠾ࡼࡧ

⃰ᗘࢆẚ㍑ࡋࡼ࠺࡜ࡋࡓ࡜ࡁࠊΰධ๭ྜࢆ▱ࡿࡇ࡜Ț⥺ ᐃ᮲௳ࡣࠊ ࠾ࡼࡧ  ࡟♧ࡋࡓ᮲௳࡜࡯

ࡀ࡛ࡁ࡞࠿ࡗࡓࡢ࡛ࠊ௒ᅇࡣࡑࡢホ౯ࢆ⾜࠺ࡇ࡜ࡀࡰྠᵝ࡞ࡢ࡛┬␎ࡍࡿࠋ

⾲ 5 ⯪㏻ᒣᆅᇦ࠿ࡽࡢ㙾㕲㖔ࡢศᯒ⤖ᯝElement 㻷㻺㻝㻙㻝
Na
56
Mg
2100
Al
2600
Cl
<36
K
3200
Ca
<180
Sc
7.6
Ti
1500
V
<0.64
Cr
46
Mn
710
Fe (%)
59
Co
8.7
Ni
<58
Zn
<16
As
<0.82
Se
<2.0
Br
<1.3
Rb
55
Zr
<220
Ag
<0.89
Sb
1.1
Te
<76
I
<4.6
Cs
1.2
Ba
<90
La
1.4
Ce
<2.2
Sm
<0.19
Tb
<0.19
Yb
0.41
Lu
<0.034
Hf
<0.44
Ta
0.24
Au
<0.0044
Th
<0.26
U
0.64
As/Sb *
䠉

㻷㻺㻝㻙㻞
360
7800
51000
110
30000
<1600
31
2400
260
<3.4
710
41
13
<58
31
2.3
<1.4
<2.5
240
100
2.3
2.3
<49
<24
6.9
310
2.0
<1.7
0.71
<0.23.
<0.18<0.038<0.43
ND
0.0038
<0.25
3.3
1.0

䠧䠪㻝㻙㻟䠝
760
<3000
35000
<140
<11000
21000
4.3
1000
29
31
620
42
250
<80
<20
11
<2.3
<3.8
65
<170
<2.7
7.4
<97
<17
2.4
<100
28
70
4.9
0.22
1.6
0.28
3.2
0.49
<0.017
5.3
4.5
1.5

(ppm)
䠧䠪㻝㻙㻟䠞 䠧䠪㻝㻙㻟䠟 䠧䠪㻝㻙㻟䠠 䠧䠪㻝㻙㻠䠝
170
270
300
520
5800
7000
9900
5100
44000
42000
61000
36000
<130
<180
<160
<110
12000
19000
22000
840
<1800
<4800
<2300
<1900
4.6
16
2.9
3.0
1100
3700
790
<340
43
220
31
33
19
53
25
24
2500
14000
1300
1300
36
21
32
38
150
13
730
480
<61
<62
<88
<78
130
75
110
130
2.5
1.1
22
16
<1.8
<1.9
2.5
<1.5
0.74
<0.88
<1.6
1.1
100
140
190
62
92
<140
<190
<170
<2.1
<2.4
<3.0
<2.6
1.2
1.8
<0.83
1.0
<73
<80
<110
<100
<17
<21
<20
<18
2.6
4.1
4.6
<0.55
250
490
560
190
22
2.6
5.2
6.9
48
6.5
12
16
3.5
0.75
0.8
1.1
<0.16
<0.21
<0.37
<0.31
1.8
<0.40
<0.54
0.94
0.25
0.099
0.078
0.15
4.2
1.5
2.7
3.6
0.41
<0.21
0.92
<0.16
<0.013<0.015<0.020<0.019
7.6
2.9
7.4
10
2.8
0.62
2.1
2.0
2.1
0.6
16.0
䠉

- 407 - ᅗ  ⯙ᓮ㑇㊧  ྕྂቡ࠿ࡽฟᅵࡢ୙᫂ᯈ≧㕲
 〇ရ㸦
㸦70㸧 ⤖ᯝཬࡧ⪃ᐹࡇࢀࡽ୙᫂ᯈ≧㕲〇ရࡢ & ⃰ᗘࡣࠊ㸣࡜㸣࡛࠶ࡾࠊ⌧௦࡛ゝ࠺పⅣ⣲㗰࡜୰Ⅳ⣲㗰࡟ᒓࡋ࡚࠸ࡓࠋ୰ᛶᏊᨺᑕ໬ศᯒࢆࡋࡓ⤖ᯝࢆ⾲ ࡟♧ࡍࠋ70 ࡣ㗵ࡧ࡚࠸ࡓࡀࠊ㯮㗵ࡢ≧ែ࡛࠶ࡾࠊ
)H ⃰ᗘࡣ 㸣࡛࠶ࡗࡓࠋ୍᪉ࠊ㔠ᒓ㒊ࢆṧࡋࡓ
70P ࡣ 㸣࡛࠶ࡗࡓࠋ㗵ࡧࡓ 70 ࡛ࡣࠊ1Dࠊ
$Oࠊ&Oࠊ. ࡢ⃰ᗘࡀ㧗࠿ࡗࡓࠋ㔠ᒓࡀṧᏑࡍࡿ 70P࡛ࡣࠊ㔠ᒓ㒊࡟⃰㞟ࡋࡸࡍ࠸ &R ࡸ $V ࡀప⃰ᗘ࡛࠶ࡗࡓࡀࠊ0R ࡸ 6E ࡀ㧗⃰ᗘ࡛࠶ࡗࡓࠋࡲࡓࠊ୧
ヨᩱ࡟ඹ㏻ࡋ࡚ =U ࡀ㧗⃰ᗘ࡛࠶ࡗࡓࠋ
㕲ཎᩱࡢ⏘ᆅ᥎ᐃࡢᣦᶆ࡜࡞ࡿ $V6E ⃰ᗘẚࢆ

3-21
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JAEA-Review 2013-039

ࡳࡿ࡜ࠊ70 ࡀ ࠊ70P ࡀ  ࡜୧ヨᩱ࡜㸵㸬ᮏ㢪ᑎቃෆ࠿ࡽฟᅵࡋࡓ㕲⁦࡜㕲ሢࡢ㛵ಀࡶ  ௨ୗࡢ್࡜࡞ࡗ࡚࠸ࡓࠋ㐣ཤࡢࢃࢀࢃࢀࡢศி㒔ࡢすᮏ㢪ᑎࡣࠊίᅵ┿᐀ࡢ᐀♽ぶ㮭⪷ேࢆ♭ᯒ⤖ᯝ࠿ࡽ᥎ ࡍࡿ࡜ࠊᮏ㕲ཎᩱࡣ᪥ᮏ⏘ࡢ㕲ཎᩱࡗࡓᮏ㢪ᑎὴࡢᮏᒣ࡛࠶ࡿࠋቃෆ࡟ࡣࠊᐶỌ  ᖺࢆ౑⏝ࡋ࡚సࡗࡓ㕲࡛ࡣ࡞ࡃࠊ㡑༙ᓥ⏘ࡢ㕲ཎᩱࢆ ᖺ ࡟ᘓ❧ࡉࢀࡓᚚᙳᇽࡀ࠶ࡾࠊᖹᡂ  ᖺ౑⏝ࡋࡓࡶࡢ࡜ᛮࢃࢀࡿࠋࡲࡓࠊ◁㕲≉᭷ࡢ 7L ࡸ 9 ᖺ ࠿ࡽᖹᡂ  ᖺ  ᖺ ࡟࠿ࡅ࡚኱つᶍ࡞⃰ᗘࡀ㠀ᖖ࡟ప⃰ᗘ࡛࠶ࡗࡓࡇ࡜࠿ࡽ㕲㖔▼࡛࠶ࡿಟ᚟ᕤ஦ࡀ⾜ࢃࢀ࡚ࡁࡓࠋࡑࡢᕤ஦ࡢ୍⎔࡛ࡣࠊᒇࡇ࡜ࡶ᥎ᐹ࡛ࡁࡓࠋ

᰿⎰ࡢ྿ࡁ᭰࠼ࡶ⾜ࢃࢀࠊ㛗ࡉ⣙ FPࠊ㔜ࡉ 㹼௨ୖࡢ⤖ᯝ࡟ࡼࡾࠊᮏヨᩱࡣ㡑༙ᓥ࠿ࡽࡢ⯧㍕ရ

J ࡢ⎰⏝㕲㔥ࡸ⿬⏥࡟␃ࡵࡿ⿬⏥⏝㕲㔥ࡀᢤࡁ࡛࠶ࡿࡇ࡜ࡀุ᫂ࡋࡓࠋ

ྲྀࡽࢀࡓࠋࡇࢀࡽࡢ㕲㔥ࡣࠊࡍ࡛࡟ศᯒࡉࢀࠊ඲࡚

ࡀྠ୍ᆅᇦ ዟฟ㞼ᆅ᪉ ࡢ◁㕲ࢆཎᩱ࡜ࡋࡓ㕲ᮦ࠿⾲  ⯙ᓮ㑇㊧ฟᅵࡢ୙᫂ᯈ≧㕲〇ရࡢࡽຍᕤࡋࡓࡶࡢ࡛࠶ࡿࡇ࡜ࡀ᫂ࡽ࠿࡜࡞ࡗ࡚࠸ࡿࠋ

㻔㼜㼜㼙㻕
TM-2m
䠘 100
Na
䠘 580
Mg
78
Al
100
Cl
䠘 34
K
䠘 980
Ca
䠘 0.084
Sc
䠘 56
Ti
䠘 0.4
V
24
Cr
㻺㻰
Mn
1000000
Fe
9.3
Co
䠘 120
Ni
䠘 25
Cu
Zn
䠘 34
8.8
Ga
11
As
䠘 0.67
Br
1600
Zr
28
Mo
䠘 0.072
In
290
Sb
䠘 3.3
I
䠘 0.80Cs
䠘 150
Ba䠘 0.063La䠘 0.46Yb䠘 0.18LuCe䠘 7.6
䠘 0.100.14
Sm䠘 0.71
䠘 1.0
Hf
0.40
䠘 0.85W䠘 0.56
䠘 0.19Dy䠘 0.006
䠘 0.0093Au䠘 0.19
0.75
Th
䠘 1.3
䠘 1.1
U
0.033
0.037
As/Sb** 䠖 Ratio of 䠝䡏 concentration to Sb concent䠘㻌䠖㻌㻸㼛㼣㼑㼞㻌㼘㼕㼙㼕㼠㻌㼛㼒㻌㼐㼑㼠㼑㼞㼙㼕㼚㼍㼠㼕㼛㼚㻺㻰䠖㻺㼛㻌㼐㼑㼠㼑㼏㼠㼑㼐௒ᅇࠊすᮏ㢪ᑎቃෆࡢ㜵⅏タഛᕤ஦࡟ࡼࡿ᥀๐ࢆ

㼑㼘㼑㼙㼑㼚㼠㼟

TM-1
750
䠘 900
1200
8500
180
䠘 1200
0.70
䠘 140
1.5
26
4
690000
6.4
䠘 91
䠘 67
䠘 27
6.6
2.7
1.7
450
22
䠘 0.2381
䠘 6.9
䠘 0.49
䠘 100
1.3
䠘 0.29
䠘 0.082䠘 5.4

⾜ࡗࡓ࡜ࡇࢁࠊ㕲㘫෬࡟㛵㐃ࡍࡿ⩚ཱྀࡸ㕲⁦ࡀฟᅵࡋࡓࠋ㕲⁦ࡢ୍ࡘ࡟ࡣࠊ኱㒊ศࡀ㕲ሢ࡛࠶ࡿヨᩱࡶฟᅵࡋࡓࠋࡇࢀࡽࡢヨᩱࡀࠊ࡝ࡢࡼ࠺࡞ᛶ᱁ࡢヨᩱ࡛࠶ࡿ࠿ࢆㄪᰝࡍࡿࡓࡵࠊ୰ᛶᏊᨺᑕ໬ศᯒࢆ⾜ࡗࡓࠋศᯒヨᩱࡢࡓࡵࡢ๓ฎ⌮ࡸ୰ᛶᏊ↷ᑕ᮲௳࠾ࡼࡧȚ⥺ ᐃ᮲௳ࡣࠊ ࠾ࡼࡧ  ࡟♧ࡋࡓ᮲௳࡜࡯
ࡰྠᵝ࡞ࡢ࡛┬␎ࡍࡿࠋ
 ⤖ᯝཬࡧ⪃ᐹ㕲⁦  Ⅼ࠾ࡼࡧ㕲ሢ  Ⅼ࡜㕲ሢ࡟㞄᥋ࡍࡿ⁦㒊࠶ࡿ࠸ࡣ㗵㒊  Ⅼࢆศᯒࡋࡓࠋ඲࡚ࡢศᯒ⤖ᯝࡣ┬␎ࡍࡿࡀࠊ㕲ཎᩱࡢ⏘ᆅ᥎ᐃࡢᣦᶆ࡜࡞ࡿ $V6E ⃰ᗘẚࡣࠊඛ࡟ศᯒࡋࡓ⎰⏝㕲㔥࠾ࡼࡧ⿬⏥⏝㕲㔥ࡢ್s ࡢ್࡜࡯ࡰ୍⮴ࡋ࡚࠸ࡓࠋᅗ  ࡣᚑ᮶ศᯒࡋ
ࡓ⎰⏝㕲㔥࡜⿬⏥⏝㕲㔥㸦‫ی‬㸧ࡢ⤖ᯝ࡜ࠊ௒ᅇศᯒ
ࡋࡓ㕲⁦㸦‫ڧ‬㸧࡜㕲ሢ ‫⤖ࡢ ۑ‬ᯝࢆᇶ࡟ࠊ⦪㍈ࢆ
6E)H ⃰ᗘẚࠊᶓ㍈ࢆ $V)H ⃰ᗘẚࡢᅗ࡟ࣉࣟࢵࢺ
ࡋࡓࡶࡢ࡛࠶ࡿࠋᅗ୰ࡢ  ᗘࡢⅬ⥺ࡣࠊ$V6E ࡢ┤⥺࡛ࠊࡇࡢⅬ⥺ୖ࡟࠶ࡿヨᩱࡣࠊ$㹱6E ⃰ᗘẚࡀ඲୍࡚ᐃࡢ  ࡛࠶ࡿࡇ࡜ࢆព࿡ࡍࡿࠋ
ࡍ࡞ࢃࡕࠊすᮏ㢪ᑎቃෆ࠿ࡽฟᅵࡋࡓ㕲㘫෬࡟㛵㐃ࡍࡿ㑇≀ࡣࠊ඲࡚㕲㔥ࡢᡂศ࡜㛵㐃ࡋ࡚࠸ࡓࠋᚚ
ᙳᇽ࡟౑⏝ࡉࢀ࡚࠸ࡓ⎰⏝㕲㔥ࡢ⥲ᮏᩘࡀࠊ࠾ࡼࡑ
 ᮏ࡛࠶ࡿࡇ࡜ࢆ⪃࠼ࡿ࡜⥲㔜㔞࡛⣙  ࢺࣥ㏆ࡃ࡟࡞ࡿࠋࡇࢀ࡟⿬⏥⏝㕲㔥ࡸ௚ࡢᘓ⠏⏝ࡢ㕲㔥ࢆ⪃࠼ࡿ࡜ྜࢃࡏ࡚ᩘࢺࣥࡢ㕲㔥ࡀ౑⏝ࡉࢀ࡚࠸ࡓ࡜ᛮ
ࢃࢀࡿࠋࡑࢀࡺ࠼ࠊᙜ᫬ ᐶỌ  ᖺ ࡢᘓ❧࡟㝿ࡋ࡚

3-21- 408 -

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JAEA-Review 2013-039

䚷䚷䚷䚷䚷䚷䚷䚷䚷䚷䚷⾲䠓䚷ศᯒヨᩱ䛾㔜㔞䚷ࡣࠊከࡃࡢ㕲ᮦࡀቃෆ࡟ᣢࡕ㎸ࡲࢀࠊࡑࡇ࡟タ⨨ࡉ▷᫬㛫↷ᑕ ヨᩱ㔜㔞䠄䡉䡃䠅ࢀࡓ㘫෬ᕤᡣ࡟ࡼࡾࠊ㕲㔥ࡢຍᕤࡀ࡞ࡉࢀ࡚࠸ࡓࡇ

㛗᫬㛫↷ᑕ ヨᩱ㔜㔞䠄䡉䡃䠅Ⲕⴥ㻺㻵㻱㻿㻙㻞㻟

㼀㻙㻞㻟
㼀㻙㻠
㼀㻙㻡
㼀㻙㻢

㻝㻤㻞㻚㻣
㻝㻝㻥㻚㻠
㻞㻜㻥㻚㻣
㻡㻞㻟㻚㻢

Ⲕⴥ㻺㻵㻱㻿㻙㻞㻟

㼀㻙㻝
㼀㻙㻞
㼀㻙㻣
㼀㻙㻤
㼀㻙㻥

㻟㻝㻣㻚㻜
㻣㻠㻟㻚㻥
㻝㻥㻠㻚㻟
㻠㻢㻞㻚㻤
㻞㻞㻝㻚㻠

㢮ఝ≀㉁

㻾㻙㻝
㻾㻙㻞
㻾㻙㻟

㻥㻥㻚㻡
㻞㻜㻝㻚㻤
㻟㻜㻝㻚㻥

㢮ఝ≀㉁

㻾㻙㻠

㻝㻠㻝㻚㻤

㼀㻣㻙㻞
㼀㻣㻙㻟

㻝㻜㻣㻚㻢
㻟㻟㻜

㼀㻣㻙㻠
㼀㻣㻙㻡

㻟㻟㻞㻚㻣
㻝㻡㻥㻚㻝

㼀㻸㻙㻝
㼀㻸㻙㻞
㼀㻸㻙㻟

㻝㻜㻠㻚㻠
㻝㻥㻡㻚㻣
㻟㻠㻣㻚㻠

㼀㻸㻙㻠

㻝㻢㻟㻚㻢

࡜ࡀఛ࠼ࡿࠋ௒ᅇฟᅵࡋࡓ㕲㘫෬࡟㛵ಀࡍࡿ⩚ཱྀࡸ㕲⁦ࡣࡑࡢ࡜ࡁ◚Რࡉࢀࡓࡶࡢࡢ୍㒊࡜ᛮࢃࢀࡿࠋ
௒ᅇࡢศᯒࡢᡂᯝ࡟ࡼࡾࠊᙜ᫬ࡢᮦᩱࡢㄪ㐩➼ࡢᵝᏊࢆ᪂ࡓ࡟▱ࡿࡇ࡜ࡀ࡛ࡁࠊ㈗㔜࡞Ⓨぢ࡜ᛮࢃࢀࡿࠋ
ẚ㍑ᶆ‽ヨᩱ
㻺㻵㻱㻿㻙㻣

㻺㻵㻿㼀㻝㻡㻣㻟㼍㻝㻚㻱㻙㻜㻠

ẚ㍑ᶆ‽ヨᩱ
㻺㻵㻱㻿㻙㻣

㻺㻵㻿㼀㻝㻡㻣㻟㼍㻝㻚㻱㻙㻜㻡
㻿㼎㻛㻲㼑㻌㻌㻌㻌⾲䠔㻌㻌㻌↷ᑕ䞉 ᐃ᮲௳䛸ศᯒඖ⣲㻵㼞㼞㼍㼐㼕㼍㼠㼕㼛㼚㻌㼒㼍㼏㼕㼘㼕㼠㼥㻘㻵㼞㼞㼍㼐㼕㼍㼠㼕㼛㼀㼔㼑㼞㼙㼍㼘㻌㼚㼑㼡㼠㼞㼛㼚㻌㼒㼘㼡㼤 㼚㻌㼠㼕㼙㼑㻙㻞㻙㻝㻌㻔㻌㼚䞉㼙 䞉㼟㼑㼏 㻕㻝㻚㻱㻙㻜㻢

㻯㼛㼛㼘㼕㼚㼓
㼠㼕㼙㼑㻯㼛㼡㼚㼠㼕㼚㼓
㼠㼕㼙㼑㻌㻭㼚㼘㼥㼦㼑㼐㻌㻌㼑㼘㼑㼙㼑㼚㼠㼟㻶㻾㻾㻙㻟㻝㻚㻱㻙㻜㻣
㻝㻚㻱㻙㻜㻢

㻝㻚㻱㻙㻜㻡

㻝㻚㻱㻙㻜㻠

㻼㻺㻙㻟䚷㻝㻚㻡㽢㻝㻜㻝㻣㻜㻚㻡㻌㼟㼑㼏 㻟㻌㼙㼕㼚䡚㻠㻌㼙㼕㼚 㻠㻜㻜䚷㼟㼑㼏 㻔㻺㼍㻕 㻹㼓 㻭㼘 㻯㼘㻯㼍 㼀㼕 㼂 㻹㼚㻯㼡 㻵 㻰㼥 㻔㻷㻕㻼㻺㻙㻝㻝㻣㻡㻚㻞㽢㻝㻜

㻝㻜㻌㼙㼕㼚

㻝㻚㻱㻙㻜㻟㻭㼟㻛㻲㼑ᅗ  すᮏ㢪ᑎᚚᙳᇽ࡟౑⏝ࡉࢀࡓ⎰⏝㕲㔥࡜⿬㻠䡚㻡㻌㼐㻞㻚㻣㻌䡄䡎㻺㼍 㻷 㻔㻭㼟㻕 㻮㼞 㻔㻹㼛㻕 㻔㻿㼎㻕㻸㼍 㻿㼙 㻔㼅㼎㻕 㻔㼁㻕 㻾㼎㻞㻜㻌㼐䡚㻞㻝㻌㼐㻞㻚㻣㻌䡄䡎㻿㼏 㻯㼞 㻲㼑 㻯㼛 㻔㻺㼕㻕 㼆㼚㻿㼎 㻮㼍 㻸㼍 㻯㼟 㻿㼙 㻔㼅㼎㻕㻔㻿㼑㻕 㻔㻴㼒㻕 㼀㼍 㼀㼔 㻔㻿㼎㻕 㻔㻮㼍㻕㻾㼎⏥⏝㕲㔥࠾ࡼࡧቃෆ࠿ࡽⓎ᥀ࡉࢀࡓ㕲⁦࡜㕲ሢࡢ $V)H ⃰ᗘẚ㸫6E)H ⃰ᗘẚࡢ┦㛵㛵ಀ ⤖ᯝ࠾ࡼࡧ⪃ᐹ㸶㸬⎔ቃᶆ‽≀㉁ೃ⿵ヨᩱ㸦Ⲕⴥϩ㸧ࡢ್௜ࡅ
㸦⊂㸧ᅜ❧⎔ቃ◊✲ᡤ㸦NIES㸧ࡣࠊከඖ⣲ศᯒࢆศᯒࡋࡓ⤖ᯝࢆࡲ࡜ࡵࡓࡢࡀ⾲  ࡛࠶ࡿࠋ⾲࡛ࡣ⾜࠺㝿ࡢ⢭ᗘ⟶⌮ࡸศᯒᶵჾࡢᰯṇࡢࡓࡵ࡟ࠊㄆド」ᩘࡢヨᩱ㸦Q 㹼㸧ࡢࢹ࣮ࢱࡢᖹᆒ್࡜ᶆ‽೫ᕪᶆ‽≀㉁ࢆᚑ᮶࠿ࡽ㛤Ⓨࡋ࡚ࡁࡓࠋ௒ᅇࠊ⎔ቃᶆ‽ࢆ♧ࡋ࡚࠸ࡿࠋ&U ࡟ࡘ࠸࡚ࡣヨᩱྡࢆ᭩ࡃ࣐ࢪࢵࢡ≀㉁ࡢ୍ࡘ࡜࡞ࡿⲔⴥᶆ‽≀㉁ೃ⿵ヨᩱ㸦NIES

࢖ࣥࢡࡢᙳ㡪ࡀฟ࡚ࡤࡽࡘࡁࡀከ࠿ࡗࡓࠋ

CRM No.23㸧ࢆ୰ᛶᏊᨺᑕ໬ศᯒࡋࡓࠋ

⾲㻥䚷⎔ቃᶆ‽≀㉁ೃ⿵䚷㻺㻵㻱㻿㻌㻯㻾㻹㻌㻺㼛㻚㻞㻟䛾ศᯒ⤖ᯝ ศᯒヨᩱศᯒヨᩱࡣࠊ⾲ 7 ࡟♧ࡍ㔜㔞ࢆ࣏࢚ࣜࢳࣞࣥ⿄࡟஧㔜ᑒධࡋࡓࠋẚ㍑ᶆ‽≀㉁ࡣࠊNIES CRM No.7
㸦Ⲕⴥ㸧࡜㏦௜ࡉࢀ࡚ࡁࡓ㢮ఝ≀㉁࡜ NIST SRM
1573a㸦ࢺ࣐ࢺ㸧ࢆ⏝࠸ࡓࠋ ୰ᛶᏊ↷ᑕ࠾ࡼࡧȚ⥺ᐃヨᩱࡢ୰ᛶᏊ↷ᑕࡣࠊJRR-3M ࡢ PN-3 ࡢẼ㏦⟶㸦▷ᑑ࿨⏝㸧࡜ PN-1 ࡢẼ㏦⟶㸦୰࣭㉸ᑑ࿨⏝㸧ࢆ౑⏝ࡋࠊヲ⣽ࢆ⾲㸶࡟♧ࡍࠋࡲࡓࠊ↷ᑕᚋࡢȚ⥺ᐃࡣ⏕ᡂࡍࡿ᰾✀ࡢ༙ῶᮇ࡟ྜࢃࡏ࡚ࠊ⾲㸶࡟♧ࡍ᮲௳࡛⾜ࡗࡓࠋ

ඖ⣲
䠩䡃
䠝䡈
䠟䡈
䠟䠽
䠩䡊
㻺㼍
㻷
㻿㼏
㻯㼞
㻲㼑
㻯㼛
㼆㼚
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ᖹᆒ್
ᶆ‽೫ᕪ 㻯㼂
䠄㼙䡃㻛㼗䡃䠅 䠄㼙䡃㻛㼗䡃䠅 䠄䠂䠅㻝㻣㻣㻜 㼼 㻤㻡㻠㻚㻤㻡㻢㻥 㼼 㻞㻞㻟㻚㻥㻥㻜㻠 㼼 㻝㻠㻝㻚㻢㻞㻤㻟㻜 㼼 㻟㻣㻟㻝㻟㻢㻥㻥 㼼 㻞㻣㻟㻚㻤㻥㻚㻞㻣 㼼 㻜㻚㻠㻠㻠㻚㻤㻞㻜㻢㻡㻜 㼼 㻟㻣㻜㻝㻚㻤㻜㻚㻜㻝㻢㻠 㼼 㻜㻚㻜㻜㻜㻟㻞㻚㻜㻜㻚㻝㻣㻜 㼼 㻜㻚㻜㻤㻣㻡㻝㻝㻜㻞 㼼 㻡㻠㻚㻢㻜㻚㻞㻞㻝 㼼 㻜㻚㻜㻝㻜㻠㻚㻢㻟㻞㻚㻣 㼼 㻝㻚㻜㻟㻚㻝㻠㻚㻣㻟 㼼 㻜㻚㻝㻝㻞㻚㻠㻝㻡㻚㻝 㼼 㻜㻚㻝㻜㻚㻤㻜㻚㻝㻝㻡 㼼 㻜㻚㻜㻝㻢㻝㻠㻜㻚㻝㻢㻤 㼼 㻜㻚㻜㻞㻜㻝㻞㻜㻚㻜㻞㻣㻠 㼼 㻜㻚㻜㻜㻝㻣㻢㻚㻟㻝㻚㻣㻞 㼼 㻜㻚㻝㻜㻡㻚㻥ศᯒᩘ ㄆド್䠄ཧ⪃್䠅㼚䠄㼙䡃㻛㼗䡃䠅
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JAEA-Review 2013-039

ᐃ㔞࡛ࡁࡓከࡃࡢඖ⣲ࡣ &9 ್ࡶᩘ㸣࡛ࡼ࠸⢭ᗘ࡛㸧 㙾㕲㖔ࢆཎᩱ࡜ࡋࡓᶍᨃࡓࡓࡽ〇㕲࠿ࡽࡢ〇㕲ศᯒࡀ⾜࠼ࡓࠋㄆド್ࡢỴᐃ࡟ࡘ࠸࡚ࡣࠊྛ✀ศᯒ㛵㐃ヨᩱࡢ⛉Ꮫⓗㄪᰝ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊ

ἲ࡟ࡼࡿඹྠศᯒ࡛⾜ࢃࢀࡓࠋ⾲  ࡟ࡣཧ⪃ࡢࡓࡵࠊࠊ1Rࠊ㸦㸧㕥ᮌ❶ᝅࠊ㕲࡜㗰ࠊᅜ❧⎔ቃ◊✲ᡤ࠿ࡽሗ࿌ࡉࢀࡓㄆド್࠾ࡼࡧཧ⪃್㸧 ⌮⛉Ꮫⓗศᯒἲ࡟ࡼࡿ⯙ᓮ㑇㊧ฟᅵࡢྂ௦㕲ᮦ

ࡶᥖ㍕ࡋࡓࠋㄆド್࡟௜ࡅࡽࢀࡓ୙☜࠿ࡉࡣࠊໟྵ

ࡢᮦ㉁ㄪᰝ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊ㕥ᮌ❶ᝅࠊಀᩘ㹩㸻 ࡢ್࡛࠶ࡿࠋཧ⪃್ࡢ 1D ࢆ㝖࠸࡚࠸ࡎࢀ

ᒸ⏣ Ꮚࠊ㕲࡜㗰ࠊࠊ1Rࠊ㸦㸧ࡶㄆド್࠶ࡿ࠸ࡣཧ⪃್࡜➼ࡋ࠿ࡗࡓࠋࡲࡓࠊᩘ್㸧 ⮬↛⛉Ꮫⓗศᯒἲ࡟ࡼࡿᮏ㢪ᑎቃෆࡼࡾฟᅵࡋ

ࡢ࡞࠸ࡶࡢࡣࠊ௚ࡢ᪉ἲ್࡛௜ࡅࡀࡉࢀ࡞࠿ࡗࡓࡶ

ࡓ㕲⁦ࡢ⛉Ꮫⓗㄪᰝ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊᮏ

ࡢ࡛࠶ࡿࠋ

㢪ᑎ㜵⅏᪋タᕤ஦࣭Ⓨ᥀ㄪᰝሗ࿌᭩ࠊ㸦㸧㸧 すᮏ㢪ᑎቃෆࡼࡾฟᅵࡋࡓ㕲⁦ཬࡧ㕲ሢࡢ㔠ᒓ㸷㸬࠾ࢃࡾ࡟ࠊᏛⓗศᯒ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊ㕲࡜㗰ࠊᩥ໬㈈㛵㐃㈨ᩱ≉࡟㕲࡟㛵ࡋ࡚ࡣࠊ㕲ཎᩱࡢ✀㢮

1Rࠊ㸦㸧ࡢྠᐃࡸ⏘ᆅࡢ᥎ᐃࡀ㠀ᖖ࡟㔜せ࡞ࡇ࡜࡜࡞ࡿࠋ୰
ᛶᏊᨺᑕ໬ศᯒ࡟ࡼࡿᚤ㔞࡞ AsࠊSbࠊTiࠊV ࡢ⃰ᗘࢆ▱ࡿࡇ࡜࡟ࡼࡾࠊࡇࢀࡽࡢၥ㢟ゎỴ࡟᭷ຠ࡟࡞

 Ⓨ⾲ࡾ࠺ࡿࠋࡑࡢࡓࡵࠊ௒ᅇሗ࿌ࡋࡓᡂᯝࡣࠊᩥ໬㈈⛉㸧 బ㈡┴཯ᑕ⅔⏤᮶ࡢ㕲㗰ศᯒ㸹ຍ⸨ᑗᙪࠊᑠ᳚
ᖾྖࠊᖹ஭᫛ྖࠊᒸ⏣ Ꮚࠊ㕥ᮌ❶ᝅࠊ㛗㔝ᭃࠊᏛࡢศ㔝࡛኱࠸࡟ᙺ❧ࡘࡶࡢ࡜☜ಙࡋ࡚࠸ࡿࠋ
ࡲࡓࠊ⎔ቃᶆ‽≀㉁ೃ⿵ࡢ್௜ࡅ࡟㛵ࡋ࡚ࡶ୰ᛶ

᪥ᮏᩥ໬㈈⛉Ꮫ఍➨  ኱఍ࠊ ᖺ  ᭶Ꮚᨺᑕ໬ศᯒࡣ┿ᗘࡀ㧗࠸ࡇ࡜࠿ࡽࠊḞ࠿ࡏ࡞࠸ศ㸧 㙾㕲㖔ࢆཎᩱ࡜ࡋࡓࡏ࠸㕲㛵㐃㈨ᩱࡢ⛉Ꮫⓗㄪᰝ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊ㕥ᮌ❶ᝅࠊᒸ⏣ Ꮚࠊᯒἲ࡛࠶ࡿࡇ࡜ࡶᐇド࡛ࡁࡓ࡜ᛮࢃࢀࡿࠋ

᪥ᮏ㕲㗰༠఍ࠕ㕲ࡢṔྐࣇ࢛࣮࣒ࣛࠖ➨  ᅇබ㛤◊✲Ⓨ⾲఍ࠊ ᖺ  ᭶㸯㸮㸬ᡂᯝࡢබ⾲㸧 ࡓࡓࡽ〇㕲ࢆゎ᫂ࡍࡿࡓࡵࡢศᯒᢏ⾡㸹ຍ⸨ᑗ ㄽᩥ➼ᙪࠊᖹ஭᫛ྖࠊ
᪥ᮏᏛ⾡᣺⯆఍〇㗰➨  ጤဨ఍ࠊ㸧 ࡲ࡯ࢁࢇ㸰ྕ⅔࡟࠾ࡅࡿ᚟ඖࡓࡓࡽ〇㕲࠿ࡽࡢ ᖺ  ᭶〇㕲㛵㐃㈨ᩱ୰ࡢඖ⣲⃰ᗘཬࡧ㔠ᒓᏛⓗ⤌⧊ࡢㄪᰝ㸹ᖹ஭᫛ྖࠊຍ⸨ᑗᙪࠊᑠ᳚ᖾྖࠊ㕥ᮌ❶㸧 ⇞↝㉥እ⥺྾཰ἲཬࡧᶵჾ୰ᛶᏊᨺᑕ໬ศᯒἲ

ᝅࠊᒸ⏣ Ꮚࠊ⚟ᓥ┴ᩥ໬㈈ࢭࣥࢱ࣮ⓑἙ㤋◊࡟ࡼࡿ᪥ᮏย୰ࡢᚤ㔞ඖ⣲ࡢᐃ㔞ࠊᒸ⏣ Ꮚࠊ

✲⣖せ ࠊ㸦㸧ᖹ஭᫛ྖࠊ኱㇂┾୍ࠊ᪥ᮏ㕲㗰༠఍➨  ᅇ᫓
Ꮨㅮ₇኱఍ࠊ ᖺ  ᭶㸧 బ㈡⸬཯ᑕ⅔⏤᮶ࡢ㕲㗰ࡢศᯒ㸹ຍ⸨ᑗᙪࠊᖹ
஭᫛ྖࠊ㕥ᮌ❶ᝅࠊᒸ⏣ Ꮚࠊᖥᮎబ㈡⛉Ꮫᢏ㸧 ᚤ㔞ඖ⣲࠿ࡽࡳࡓᘺ⏕ࡢ㕲㸹ᖹ஭᫛ྖࠊ᪥ᮏ㕲㗰༠఍ࠕ㕲ࡢṔྐࣇ࢛࣮࣒ࣛࠖ➨  ᅇࣇ࢛࣮ࣛ

⾡ྐ◊✲ ➨  ྕࠊ㸦㸧࣒ㅮ₇఍㸧 బ㈡⠏ᆅཬࡧከᕸ᪋཯ᑕ⅔㊧ᆅ࠿ࡽⓎ᥀ࡉࢀࡓ㕲ཬࡧࢫࣛࢢࡢศᯒ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊᒸ㸧 すᮏ㢪ᑎቃෆ࠿ࡽฟᅵࡋࡓ㕲⁦࡜ᚚᙳᇽࡢ㕲㔥⏣ Ꮚࠊ㕥ᮌ❶ᝅࠊ㛗㔝ᭃࠊ⪃ྂᏛ࡜⮬↛⛉Ꮫࠊ࡜ࡢ㛵ಀ㸹ᖹ஭᫛ྖࠊຍ⸨ᑗᙪࠊᒸ⏣ Ꮚࠊ᪥ࠊ㸦㸧ᮏᩥ໬㈈⛉Ꮫ఍➨  ᅇ኱఍ࠊ ᖺ  ᭶㸧 ㇏ᓥ༊ᕢ㬞㑇㊧ཬࡧᰁ஭㑇㊧ฟᅵࡢ㕲㔥ࡢ⮬↛㸧 $V6E ⃰ᗘẚࢆᣦᶆ࡜ࡋࡓすᮏ㢪ᑎࡢ㕲㔥ཬࡧ⛉Ꮫⓗศᯒ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊ㇏ᓥ༊ᇙⶶ

㕲⁦ࡢཎᮦᩱࡢ⏘ᆅ᥎ᐃ㸹ຍ⸨ᑗᙪࠊᖹ஭᫛ྖࠊ

ᩥ໬㈈ㄪᰝሗ࿌  ᕢ㬞⏫ ;,,ࠊࠊ෗┿᪥ᮏᩥ໬㈈⛉Ꮫ఍➨  ᅇ኱఍ࠊ ᖺ  ᭶

3-21

ᅗ∧ ෗┿ᅗ∧ 㸦㸧

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JAEA-Review 2013-039

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4. Others- 411 -

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JAEA-Review 2013-039

4-1⎇ⓥ࠹࡯ࡑ㧦ࡈࠖ࠶࡚ࠪࡦ࠻࡜࠶ࠢᴺߦࠃࠆⅣႺ⹜ᢱਛߩᩭ‛⾰ᬌ಴
⴫   㗴㧦ࡈࠖ࠶࡚ࠪࡦ࠻࡜࠶ࠢᴺߩ଻㓚ភ⟎ⅣႺ⹜ᢱࡄ࡯࠹ࠖࠢ࡞ಽᨆ߳ߩᔕ↪

଻㓚ភ⟎ⅣႺ⹜ᢱߩߚ߼ߩ㜞Ớ❗࠙࡜ࡦࠍ฽߻☸ሶߩㆬᛯ⊛ㆬ಴᧘ ⥌࿻‫ޔ‬㋈ᧁᄢテ‫ޔ‬ᳯဈᢥቁ‫ޔ‬㑆ᨩᱜ᣿‫⾆᧛ᧁޔ‬ᶏ‫◉ޔ‬ේિᄦᣣᧄේሶജ⎇ⓥ㐿⊒ᯏ᭴ ේሶജၮ␆Ꮏቇ⎇ⓥㇱ㐷 ⅣႺ࡮ේሶജᓸ㊂ಽᨆ⎇ⓥࠣ࡞࡯ࡊ଻㓚ភ⟎ⅣႺ⾗ᢱᴺߪ‫ޔ‬ේሶജ㑐ㅪᣉ⸳ฦỚ❗ᐲߩ☸ሶ߇ᬌ಴ߐࠇࠆࠛ࠶࠴ࡦࠣᤨ

߆ࠄណ㓸ߒߚࠬࡢࠗࡊ⹜ᢱਛߦ฽߹ࠇࠆᩭ

㑆ࠍ᳿߼ࠆᔅⷐ߇޽ࠆ‫ޕ‬࿑ 1 ߪ㧘⒳‫ߩޘ‬Ớ❗

ಽⵚᕈ‛⾰ߩห૏૕Ყࠍ᷹ቯߔࠆߎߣߦࠃ

ᐲߩ࠙࡜ࡦ☸ሶߦኻߒߡ㧘45͠ߩ 1M NaOHࠅᧂ↳๔ේሶജᵴേߩᬌ⍮ࠍ⋡⊛ߣߒߚ‫ޔ‬ߩࠛ࠶࠴ࡦࠣ᧦ઙߢ㧘FTࠍᬌ಴ߔࠆߚ߼ߦ

IAEAߩ଻㓚ភ⟎ߩᒝൻ╷ߣߒߡዉ౉ߐࠇߚ

ᔅⷐߥࠛ࠶࠴ࡦࠣᤨ㑆ߩ࠙࡜ࡦ☸ሶߩỚ❗

߽ߩߢ޽ࠆ‫⹜ࡊࠗࡢࠬޕ‬ᢱ߆ࠄ࿁෼ߒߚ୘‫ޘ‬ᐲଐሽᕈࠍ␜ߔ‫ޕ‬Ớ❗ᐲߩჇടߣ౒ߦߘߩࠛ

ߩ☸ሶߩห૏૕Ყࠍ᷹ቯߔࠆࡄ࡯࠹ࠖࠢ࡞

࠶࠴ࡦࠣᤨ㑆߇⍴ߊߥࠆߎߣ߇ಽ߆ࠆ‫ޕ‬࿑ 1ಽᨆߢߪ࿁෼ߐࠇߚήᢙߩ☸ሶߩਛߢ⇼޿ߩ㑐ଥߦၮߠ޿ߡ㧘☸ᓘಽᏓ߇ 0.8㨪3 Pmߩߩ޽ࠆ☸ሶ߇௖߆ߦሽ࿷ߔࠆ႐วߢ߽‫ࠇߘޔ‬10%Ớ❗࠙࡜ࡦߣᄤὼ⚵ᚑߩ࠙࡜ࡦ☸ሶࠍࠍ⏕ታߦᬌ಴ߔࠆᔅⷐ߇޽ࠆ‫ޕ‬FT-TIMSᴺߦ

ᷙวߒߚ⹜ᢱࠍ⺞⵾ߒ㧘10%Ớ❗࠙࡜ࡦࠍఝ

ࠃࠆࡄ࡯࠹ࠖࠢ࡞ಽᨆߢߪ‫ࠨࡦࡠࠢࡒࡉࠨޔ‬వ⊛ߦᬌ಴ߔࠆታ㛎ࠍⴕߞߚ‫ޕ‬ᬌ಴ེߩࠛ࠶

ࠗ࠭ߩ☸ሶߦኻߒߡ߽㜞ᗵᐲߥᬌ಴ߣಽᨆ

࠴ࡦࠣᴺߪ 2 Ბ㓏ࠛ࠶࠴ࡦࠣᴺࠍ↪޿㧘ࠛ࠶

1)߇น⢻ߢ޽ࠆ‫⎇ᧄ ޕ‬ⓥߢߪ଻㓚ភ⟎਄㊀ⷐߥ

࠴ࡦࠣ㧙1 ߢ☸ᓘߩᄢ߈޿ 10%Ớ❗࠙࡜ࡦࠍ㜞޿Ớ❗ᐲߩ࠙࡜ࡦ☸ሶࠍ‫ޔ‬FTࠍᬌ಴ߔࠆߚ

ᬌ಴ߒ㧘ࠛ࠶࠴ࡦࠣ㧙2 ߢ☸ᓘߩዊߐ޿ 10%߼ߩࠛ࠶࠴ࡦࠣᤨ㑆╬ߩ೙ᓮߦࠃࠅ‫⾰ޔ‬㊂ಽᨆ

Ớ❗࠙࡜ࡦࠍᬌ಴ߔࠆ‫ࠣࡦ࠴࠶ࠛޕ‬㧙1 ߢߩࠛ࠶࠴ࡦࠣᤨ㑆ߪ㧘10%Ớ❗࠙࡜ࡦߩߺ߇ᬌ

FTߪᾲਛᕈሶᾖ኿ߦࠃࠅ࠙࡜ࡦ☸ሶߩ৻ㇱ߇ᩭಽⵚߒߚ㓙↢ᚑߔࠆᩭಽⵚ

಴ߐࠇࠆ 100 ಽࠍ↪޿ߚ‫ޕ‬࿑ 2 ߦ 100 ಽߩࠛߩ㘧〔ߢ޽ࠅ㧘࠙࡜ࡦ☸ሶࠍ᭴ᚑߒߡ޿ࠆ࠙࡜ࡦ
ห૏૕ߩਛߢᩭಽⵚ߇⿠߈߿ߔ޿ߩߪ

235

U

235

ߩߺߢ޽ࠆߩߢ㧘 Uߩ฽᦭㊂߇ᄙ޿㜞Ớ❗
ᐲ☸ሶ߶ߤFT߇ᄙߊߥࠆ‫ޕ‬FTߩࠛ࠶࠴ࡦࠣ
ㅦᐲߪ☸ሶߩỚ❗ᐲߩჇടߣ౒ߦㅦߊߥࠆ‫ޕ‬
3)ߎࠇߪ㧘㜞Ớ❗ᐲߩ☸ሶ߶ߤ⍴޿ࠛ࠶࠴ࡦ

ࠣᤨ㑆ߢᬌ಴ߐࠇࠆߎߣࠍᗧ๧ߒ㧘ࠛ࠶࠴ࡦ100䉡䊤䊮☸ሶ䈱Ớ❗ᐲ (%)ߩ೨ߦᬌ಴ߢ߈ࠆᣇᴺࠍ㐿⊒ߒߚ‫ޕ‬

2)࡜ࡦ☸ሶࠍFTᬌ಴ེߩࠛ࠶࠴ࡦࠣᤨ㑆ߩ೙ᓮߦࠃࠅỚ❗ᐲ೎ߦᬌ಴ߔࠆߚ߼ߦߪ㧘߹ߕ

䊶1M NaOH, 45 㷄䊶Particle diameter㩷㩷㩷~ 㪊㩷Pm

60
40

35%

20

10%

5%

0
20

ࠣᤨ㑆ࠍ೙ᓮߔࠆߎߣߦࠃࠅ࠙࡜ࡦ☸ሶߩỚ❗ᐲ೎ᬌ಴߇น⢻ߢ޽ࠆߎߣ␜ໂߔࠆ‫࠙ޕ‬

85%

80

40

60

80

100

120

NU
140

䉣䉾䉼䊮䉫ᤨ㑆㩷㪆ಽ࿑㧝 ⒳‫ߩޘ‬Ớ❗ᐲߩ࠙࡜ࡦ☸ሶߦ߅ߌࠆ‫ޔ‬FT߇ᬌ಴ߐࠇࠆ߹ߢߩࠛ࠶࠴ࡦࠣᤨ㑆ߩỚ❗ᐲଐሽᕈ‫ޕ‬ ේሶἹ㧦JRR-3     ⵝ⟎㧦᳇ㅍ▤    ಽ㊁㧦ߘߩઁ㧔ࡈࠖ࠶࡚ࠪࡦ࠻࡜࠶ࠢ㧕- 413 -

JAEA-Review 2013-039

࠶࠴ࡦࠣߦࠃࠅᬌ಴ߐࠇߚFTᒻ⁁ߩ଀ߣ㧘ࠆ‫ߦ⥸৻ޕ‬㧘FTߩᢙ߇ห⒟ᐲߢ޽ࠇ߫㧘☸

ߘࠇߦኻᔕߔࠆ࠙࡜ࡦ☸ሶߩห૏૕Ყ᷹ቯ

ᓘ߇ዊߐ޿ᣇ߇㜞Ớ❗ߢ޽ࠆ‫ࠍ଀ߩߘޕ‬࿑ 3⚿ᨐࠍ␜ߔ‫ޕ‬࿑ߦ␜ߒߚࠃ߁ߦ㧘ࠛ࠶࠴ࡦࠣ

ߦ␜ߒߚ‫ޕ‬FTᒻ⁁߇ห⒟ᐲߢࠇ߫㧘☸ᓘߩ

㧙1 ߦࠃࠅᬌ಴ߐࠇߚ࠙࡜ࡦ☸ሶߪߔߴߡ

ዊߐ޿☸ሶߪ 10%Ớ❗࠙࡜ࡦ㧘☸ᓘߩᄢ߈޿

10%Ớ❗࠙࡜ࡦߢ޽ࠆߎߣ߇⏕⹺ߐࠇߚ‫⛯ޕ‬☸ሶߪᄤὼ࠙࡜ࡦߢ޽ࠆߎߣ߇⏕⹺ߢ߈ࠆ‫ޕ‬޿ߡߩࠛ࠶࠴ࡦࠣ㧙2 ߢߪ㧘ߔߴߡߩ࠙࡜ࡦ

ߎߩࠃ߁ߦ㧘㜞޿Ớ❗ᐲߩ࠙࡜ࡦ☸ሶࠍ☸ሶ߇ᬌ಴ߐࠇࠆ᧦ઙߢ޽ࠆߩߢ㧘FTᒻ⁁☸ᓘᲤߦ 2 ࿁ߦࠊߚߞߡᬌ಴ߔࠆߩߢ㧘ᬌ಴ߛߌߢߪਔ⠪඙೎ߪ࿎㔍ߢ޽ࠆ‫ޕ‬හߜ㧘☸ᓘല₸ߪ㜞ߊߥࠆ‫ߦ․ޕ‬㧘ࠬࡢࠗࡊ⹜ᢱ߆ࠄ࿁

ߩዊߐ޿ 10%Ớ❗࠙࡜ࡦߣ☸ᓘߩᄢ߈޿ᄤ

෼ߒߚήᢙߩ࠙࡜ࡦ☸ሶߩਛߦ㜞Ớ❗ᐲ࠙ὼ࠙࡜ࡦߩ႐ว㧘෺ᣇߩFTᒻ⁁ߪ㘃ૃߔࠆ࡜ࡦ߇ࠊߕ߆ߦሽ࿷ߔࠆ႐วߢ߽㧘ߘࠇࠍ⷗႐ว߇޽ࠆߩߢ඙೎ߢ߈ߥ޿‫ߥ߁ࠃߩߎޕ‬႐ㅏߐߕ⷗ߟߌ಴ߔߎߣ߇ߢ߈ࠆ‫ޕ‬วߪ㧘FTߦኻᔕߔࠆ☸ሶߩᄢ߈ߐࠍᲧセߔෳ⠨ᢥ₂1) C. G. LEE et al., Jan. J. Appl. Phys. 42 (2006)
L1121-L1123.

2) C. G. LEE et al., J. Nucl. Sci. Techol., 46 (2009)809-813.

10% U

10% U

NU

NU

3) C. G. LEE et al., NIMB 245 (2006) 440-444.

(a)1.3 10 -1

(b)
20 Pm

1.2 10 -1

20 Pm

(a)
0.1286235 U/ 238 U

1.1 10 -1

(b)

235

U/ 238U

0.12360.1186
0.1136

10% enriched U(certified value: 0.1136)

1.0 10 -1

NU(7.25 x 10 -3㩷)

9.0 10 -3

7.0 10 -3

0.1086

10% enriched U(certified value: 0.1136)

5.0 10 -3

0.1036

0

1

2

3

4

5

6

7

8

9

10 11

☸ሶ⇟ภ
0

1

2

3

4

5

6

7

8

9

10

☸ሶ⇟ภ

࿑ 3 ࠛ࠶࠴ࡦࠣ࡯2 ߦࠃࠅᬌ಴ߐࠇߚ FT㧔a㧕࿑ 2 ࠛ࠶࠴ࡦࠣ࡯㧝ߦࠃࠅᬌ಴ߐࠇߚ FT㧔a㧕ߣߘࠇߦኻᔕߔࠆ࠙࡜ࡦ☸ሶߩห૏૕Ყ᷹ቯ⚿ᨐ㧔b㧕ߣߘࠇߦኻᔕߔࠆ࠙࡜ࡦ☸ሶߩห૏૕Ყ᷹ቯ⚿ᨐ㧔b㧕‫ޕ‬࿑(a)ਛߩࠬࠤ࡯࡞ߪ 10 Pm ߢ޽ࠆ‫ޕ‬4-1- 414 -

JAEA-Review 2013-039

お わ り に
本報告書は、研究炉（JRR-3、JRR-4）を利用した利用者の協力を基に、研究炉の成果を提出して頂き、研究炉利用課で編集したものであります。この成果を公表する事で、研究炉の今後の有効利用並びに利用拡大に役立つ事を期待します。

編集委員

編集委員メンバー
笹島文雄（研究炉利用課長）

高橋広幸（研究炉利用課）

大和田博之（研究炉利用課）- 415 -

JAEA-Review 2013-039

謝辞

本報告書の発刊にあたり、多くの皆様から多大なご協力を頂きました。
原稿を提出して頂いた利用者の皆様のご協力に感謝するとともに、今後も研究炉が有効に利用され、種々の研究がさらに進展されることを期待します。
編集に際し、ご協力頂いた、研究炉加速器管理部長 丸尾毅氏、研究炉加速器管理部
JRR-4管理課課長 木名瀬政美氏に深く感謝致します。

- 416 -

JAEA-Review 2013-039


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௜ 㘓


Appendixes- 417 -

This is a blank page.

JAEA-Review 2013-039

付 録

原科研研究炉の利用設備一覧
１．ＪＲＲ－３
１）実験設備
実 験 孔
１Ｇ
１Ｇ－Ａ
１Ｇ－Ｂ
２Ｇ
３Ｇ
４Ｇ
５Ｇ
６Ｇ
７Ｒ
Ｔ１－１
Ｔ１－２
Ｔ１－３
Ｔ１－４－１
Ｔ１－４－２
Ｔ１－４－３Ｔ１－４－４Ｔ１－４－５
Ｔ２－１
Ｔ２－２
Ｔ２－３
Ｔ２－４
Ｃ１－１
Ｃ１－２
Ｃ１－３
Ｃ２－１
Ｃ２－２
Ｃ２－３－１Ｃ２－３－２－１
Ｃ２－３－２－２
Ｃ２－３－３－１
Ｃ２－３－３－２
Ｃ２－３－３－３
Ｃ２－３－３－４
Ｃ３－１－１Ｃ３－１－２－１
Ｃ３－１－２－２
Ｃ３－２
E

実
験
装
置
高分解能粉末中性子回折装置（ＨＲＰＤ）
生体高分子用中性子解析装置（ＢＩＸ－Ⅲ）
生体高分子用中性子解析装置（ＢＩＸ―Ⅳ）
三軸型中性子分光器（ＴＡＳ－１）
中性子トポグラフィ及び精密光学実験装置（ＰＮＯ）
汎用三軸型中性子分光器（ＧＰＴＡＳ）
偏極中性子散乱装置（ＰＯＮＴＡ）
東北大学中性子散乱分光器（ＴＯＰＡＮ）
中性子ラジオグラフィ装置（ＴＮＲＦ）
中性子偏極回折装置（ＨＱＲ）
単結晶中性子回折装置（ＫＳＤ）
粉末中性子回折装置（ＫＰＤ）
即発ガンマ線分析装置（ＰＧＡ）
多重即発ガンマ線分析装置（ＭＰＧＡ）
ＴＯＦ型中性子反射率計（ＴＯＦ）
中性子ラウエ回折装置（ＬＡＵＥ）
中性子ベータ崩壊基礎測定装置
残留応力測定中性子回折装置（ＲＥＳＡ）
中性子４軸回折装置（ＦＯＮＤＥＲ）
多目的単色熱中性子ビームポート（ＭＵＳＡＳＨＩ）
高分解能三軸型中性子分光器（ＴＡＳ－２）
高エネルギー分解能三軸型中性子分光器（ＨＥＲ）
二次元位置測定小角散乱装置（ＳＡＮＳ－Ｕ）
超高分解能後方散乱装置（ＵＬＳ）
冷中性子散乱実験デバイス開発装置（ＬＴＡＳ）
高Ｑ領域対応中性子反射率計（ＳＵＩＲＥＮ）
中性子スピンエコー分光器（ＮＳＥ）
多重即発ガンマ線分析装置（ＭＰＧＡ）
即発ガンマ線分析装置（ＰＧＡ）
冷中性子ラジオグラフィ（ＣＮＲＦ）
パルス中性子機器開発装置（ＣＨＯＰ）
ＴＯＦ型中性子反射率計（ＴＯＦ）
中性子ラウエ回折装置(ＬＡＵＥ)
高分解能パルス冷中性子分光器（ＡＧＮＥＳ）
中性子光学システム評価装置（ＮＯＰ）
多層膜中性子干渉計／反射率計（ＭＩＮＥ）
中性子小角散乱装置（ＳＡＮＳ－Ｊ）
A

E- 419 -

JAEA-Review 2013-039２）照射設備
水 力 照 射 設 備
AＨＲ－１,２A気 送 照 射 設 備

E

ＰＮ－１,２E

放射化分析用照射設備

A

均 一 照 射 設 備

ＰＮ－３
ＳＩ－１

A

回 転 照 射 設 備

E

垂 直 照 射 設 備
A

ＤＲ－１
E

E

ＶＴ－１,ＲＧ－１～４
ＢＲ－１～４,ＳＨ－１

２．ＪＲＲ－４
１）実験設備プ
AールE

中性子ビーム設備
散 乱 実 験 設 備
AE

冷却水循環ループ
医療照射設備（ＢＮＣＴ）
即発ガンマ線分析装置
２）照射設備Ｔパイプ（水力）Ｓパイプ
簡 易 照 射 筒
A

E

Ｄパイプ
Ｎパイプ
気送管照射設備

ＰＮ- 420 -

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