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川崎 卓郎; 高橋 美和子*; 鬼柳 亮嗣; 大原 高志
Acta Crystallographica Section C; Structural Chemistry (Internet), 78(12), p.743 - 748, 2022/12
被引用回数：0 パーセンタイル：0.02(Chemistry, Multidisciplinary)Structural changes of the raffinose crystal on dehydration from the pentahydrate to the tetrahydrate were investigated by single-crystal time-of-flight neutron diffraction. It was revealed that during the dehydration, rearrangement occurs in the hydrogen bonds related to the lost water molecule, while the symmetry of the crystal structure is retained. The hydrogen-bonding status of raffinose pentahydrate and tetrahydrate were discussed comprehensively according to Jeffrey's hydrogen-bonding classification. It was shown that water molecules are hydrogen bonded to the surrounding molecules by 
O-H...O hydrogen bonds and 
C-H...O hydrogen bonds, and the number of these two types of hydrogen bonds determines the water molecules that are removed by dehydration. The lattice constant c showed a significant decrease on dehydration and further dehydration leads to loss of crystallinity of the raffinose crystals.
At]NaAt and [
I]NaI in an NIS-expressing thyroid cancer mouse model渡部 直史*; Liu, Y.*; 兼田 加珠子*; 佐藤 達彦; 白神 宜史*; 大江 一弘*; 豊嶋 厚史*; 下瀬川 恵久*; Wang, Y.*; 羽場 宏光*; et al.
International Journal of Molecular Sciences (Internet), 23(16), p.9434_1 - 9434_11, 2022/08
被引用回数：2 パーセンタイル：78.6(Biochemistry & Molecular Biology)
線放出核種であるAt-211(At)は、甲状腺がん治療に従来使われてきた
線放出核種であるIよりも高い治療効果を有することが期待されている。そこで本研究では、担癌マウスを用いた動物実験、及びK1-NIS細胞を用いたDNA損傷収率及び細胞生存率測定を実施し、AtとIの効果の違いを検証した。その結果、いずれの実験においてもAtの方が高い効果があることが認められた。
村瀬 清華*; 片岡 龍峰*; 西山 尚典*; 西村 耕司*; 橋本 大志*; 田中 良昌*; 門倉 昭*; 冨川 喜弘*; 堤 雅基*; 小川 泰信*; et al.
Journal of Space Weather and Space Climate (Internet), 12, p.18_1 - 18_16, 2022/06
被引用回数：0 パーセンタイル：0.01(Astronomy & Astrophysics)巨大な太陽フレアによってもたらされる太陽風により磁気圏内にエネルギーが溜まり、そのエネルギーが一気に解放されるサブストームが発生する。そのサブストームが発生する際、高エネルギー電子が大量に中間圏まで降り注ぐ事象(EEP)がしばしば観測されるが、その詳細な発生メカニズムは解明されていない。本研究では、あらせ衛星により観測された2つのEEPに対して、3次元グローバル電磁流体力学的(MHD)シミュレーションや放射線挙動解析コードPHITSを使った解析によりその発生メカニズムを検討した。その結果、カレントシート散乱とwave-particle散乱がEEPの初期及びサブストーム発生後に重要な役割を果たしていることが示唆された。
大原 高志
日本結晶学会誌, 64(2), p.132 - 139, 2022/05
中性子を用いる単結晶中性子回折法は原子核の位置を直接観察できることに加えて水素原子に対する感度が高いことから、結晶中の水素原子位置を高精度で確実に観察できる強力な手法となる。日本国内では1990年代末からJRR-3研究用原子炉を中心に単結晶中性子回折計の開発が進み、金属錯体など格子体積の比較的大きい分子性結晶における水素原子の観察が現実的になるとともに、より大強度の中性子源であるJ-PARCの建設が始まった。そのなかで筆者は単結晶中性子回折計の開発と並行して、単結晶中性子構造解析による分子性結晶中の水素原子の確実な観察を基にした研究を展開してきた。本稿では、これらの水素原子が鍵となる研究について概説する。
寺澤 有果菜*; 大原 高志; 佐藤 宗太*; 吉田 知史*; 朝日 透*
Acta Crystallographica Section E; Crystallographic Communications (Internet), 78(3), p.306 - 312, 2022/03
Precise single-crystal structure analyses of the title compound, nondeuterated triglycine sulfate (HTGS) at 20 K and 298 K were undertaken using time-of-flight neutron diffraction data. At 20 K for the O-H...O hydrogen bond between the glycinium cation and the zwitterionic, unprotonated glycine molecule that is associated with the ferroelectric behaviour of HTGS. Two reasonable structures for the same three atoms were refined for the 298 K dataset. One is a single-minimum potential-energy model, having the H atom with a large ellipticity along the bond path between the O atoms. The other is a double-minimum potential-energy model having two H atom sites with occupancies of 0.876 and 0.124.
山下 恵史朗*; 小松 一生*; 大原 高志; 宗像 孝司*; 入舩 徹男*; 新名 亨*; 杉山 和正*; 川又 透*; 鍵 裕之*
High Pressure Research, 42(1), p.121 - 135, 2022/03
被引用回数：1 パーセンタイル：63.35(Physics, Multidisciplinary)We improved diamond anvil cells with a tubular frame made of Zr-based bulk metallic glass and nano-polycrystalline diamond anvils for single-crystal neutron diffraction. The thicker tubular frame was confirmed through experimentation as stably generating 4.5 GPa. Its feasibility for neutron diffraction was assessed at the Laue-TOF diffractometer at the BL18 (SENJU) beamline in the MLF J-PARC using time-resolved two-dimensional detectors covering wide solid angles. In addition to ambient-pressure measurements of NH
Cl, diffraction patterns of a high-pressure phase of ice were also collected in-situ. The obtained intensities are of refinable quality sufficient for structure analysis.
矢野 喜男*; 小野 利和*; 大原 高志; 久枝 良雄*
Chemistry; A European Journal, 27(71), p.17802 - 17807, 2021/12
被引用回数：1 パーセンタイル：15.16(Chemistry, Multidisciplinary)X-ray diffraction, neutron diffraction, and Hirshfeld atom refinement (HAR) demonstrate that the slight difference of the N...H...O hydrogen bonds (HBs) in crystalline metastable acid-base complexes gives distinct photoluminescent properties. Our results contribute to understanding the complicated relationship between photofunction and proton dynamics in acid-base complexes, helping to create novel photofunctional materials.
中村 龍也; 藤 健太郎; 小泉 智克; 鬼柳 亮嗣; 大原 高志; 海老根 守澄; 坂佐井 馨
Proceedings of 2020 IEEE Nuclear Science Symposium and Medical Imaging Conference (NSS/MIC 2020), Vol.1, p.483 - 484, 2021/09
J-PARCに設置されたSENJU回折計に増設するためのコンパクトな2次元シンチレータ中性子検出器を開発した。本検出器では設置部の空間制約に対応するため、オリジナルと同様の有感面積(256
256mm)とピクセル分解能(44mm)を保持しつつ、奥行き170mm(従来比40%減)へ再設計し製作した。また、新開発のコンパレータボードを装填することでPMT印加電圧の低減と計数均一性を改善した。4台製作した増設用検出器はいずれも検出効率50-60% (2
)、
Coガンマ感度110
、計数均一性3-6%であり良好な性能を有することを確認した。
金子 耕士; 川崎 卓郎; 仲村 愛*; 宗像 孝司*; 中尾 朗子*; 花島 隆泰*; 鬼柳 亮嗣; 大原 高志; 辺土 正人*; 仲間 隆男*; et al.
Journal of the Physical Society of Japan, 90(6), p.064704_1 - 064704_6, 2021/06
被引用回数：23 パーセンタイル：95.74(Physics, Multidisciplinary)Multiple transition phenomena in divalent Eu compound EuAl with the tetragonal structure were investigated via single crystal time-of-flight neutron Laue technique. At 30 K below a charge-density-wave (CDW) transition, superlattice peaks emerge near nuclear Bragg peaks described by an ordering vector 
= (0 0 
). In contrast, magnetic peaks appear at 
with 
= 0.09 below 
= 15.4 K, and moves to 
with 
= 0.19 below 
=12.2 K, whereas no distinct change in the magnetic Bragg peak was detected at 
and 
. The structural modification with is characterized by an absence of the superlattice peak in (0 0 
). Considering an absence of splitting in magnetic peaks along , the structural transition is mainly ascribed to a displacement of Al ions within the tetragonal 
-plane. Complex incommensurate magnetic transitions are in stark contrast to a simple collinear commensurate structure in isovalent EuGa. This could stem from incompatible electronic structures with the CDW transition between two compounds.
松本 貴裕*; 杉本 秀彦*; 大原 高志; 徳光 昭夫*; 冨田 誠*; 池田 進*
Physical Review B, 103(24), p.245401_1 - 245401_9, 2021/06
被引用回数：0 パーセンタイル：0(Materials Science, Multidisciplinary)We investigate the quantum entangled state of two protons terminating on a silicon surface. The entangled states were detected using the surface vibrational dynamics of nanocrystalline silicon with inelastic neutron scattering spectroscopy. The protons are identical, therefore the harmonic oscillator parity constrains the spin degrees of freedom, forming strongly entangled states for all the energy levels of surface vibrations. Compared to the proton entanglement previously observed in hydrogen molecules, this entanglement is characterized by an enormous energy difference of 113 meV between the spin singlet ground state and the spin triplet excited state. We theoretically demonstrate the cascade transition of terahertz entangled photon pairs utilizing proton entanglement.
松本 貴裕*; 野又 郁実*; 大原 高志; 金光 義彦*
Physical Review Materials (Internet), 5(6), p.066003_1 - 066003_9, 2021/06
被引用回数：0 パーセンタイル：0(Materials Science, Multidisciplinary)The hydrogen isotope deuterium has attracted special interest for the manufacture of silicon (Si) semiconductors as well as for the synthesis of isotopically labeled compounds. However, the efficient production of D or H deuteride in a controlled manner is challenging, and rational H isotope enrichment protocols are still lacking. Here, we demonstrate a highly efficient exchange reaction from H to D on the surface of nanocrystalline Si. Fourfold enrichment of D termination was successfully achieved by dipping n-Si into a dilute D solution. By determining the surface-localized vibrational modes for H-and D-terminated n-Si using inelastic neutron scattering spectroscopy, we found that the physical mechanism responsible for this enrichment originates from the difference in the zero-point oscillation energies and entropies of the surface-localized vibrations.
Kwon, H.*; Pietrasiak, E.*; 大原 高志; 中尾 朗子*; Chae, B.*; Hwang, C.-C.*; Jung, D.*; Hwang, I.-C.*; Ko, Y. H.*; Kim, K.*; et al.
Inorganic Chemistry, 60(9), p.6403 - 6409, 2021/05
被引用回数：0 パーセンタイル：0.01(Chemistry, Inorganic & Nuclear)The synthesis of sandwich-shaped multinuclear silver complexes with planar penta- and tetranuclear wheel-shaped silver units and a central anion is reported, along with complete spectroscopic and structural characterization. An NMR mechanistic study reveals that silver complexes were formed in the following order: 2Ag 
3Ag
5Ag
4Ag. The central hydroxides in 4Ag and 5Ag exhibit exotic physical properties due to the confined environment inside the complex. The size of these silver wheels can be tuned by changing the central anion or extracting/adding one silver atom. This study provides the facile way to synthesize discrete wheel-shaped multinuclear silver complexes and provides valuable insights into the dynamics of the self-assembly process.
GeP
S
矢島 健*; 日沼 洋陽*; 堀 智*; 岩崎 類*; 菅野 了次*; 大原 高志; 中尾 朗子*; 宗像 孝司*; 廣井 善二*
Journal of Materials Chemistry A, 9(18), p.11278 - 11284, 2021/05
被引用回数：10 パーセンタイル：79.18(Chemistry, Physical)Herein, we studied the crystalline compound LiGePS with the largest Li-ion conductivity thus far via a novel route based on a combination of single-crystal neutron diffraction experiments at low temperature and first-principles calculations, and found that a correlated migration of the densely packed Li ions governs the overall Li-ion conduction. The correlated migration mechanism provides us with guidelines on how to design efficient superionic conductors for more efficient batteries.
三浦 大輔*; 熊田 高之; 関根 由莉奈; 元川 竜平; 中川 洋; 大場 洋次郎; 大原 高志; 高田 慎一; 廣井 孝介; 森川 利明*; et al.
Journal of Applied Crystallography, 54(2), p.454 - 460, 2021/04
被引用回数：1 パーセンタイル：29.8(Chemistry, Multidisciplinary)山形大学が原子核物理実験用に開発した結晶試料の核スピン偏極技術を、スピンコントラスト偏極中性子回折測定法に展開し、水素核偏極化されたグルタミン酸を用いて粉末結晶試料中の水素の配向および凝集・分散などの構造情報を抽出できることを実証した。
阿部 雄太; 土川 雄介; 甲斐 哲也; 松本 吉弘*; Parker, J. D.*; 篠原 武尚; 大石 佑治*; 加美山 隆*; 永江 勇二; 佐藤 一憲
JPS Conference Proceedings (Internet), 33, p.011075_1 - 011075_6, 2021/03
Since the hardness of fuel debris containing boride from BC pellet in control rod is estimated to be two times higher as that of oxide, such as UO and ZrO, distribution of such boride in the fuel debris formed in the Fukushima-Daiichi Nuclear Power Plants may affect the process of debris cutting and removal. The high neutron absorption of boron may affect the possibility of re-criticality during the process of debris removal. Therefore, boride distribution in fuel debris is regarded as an important issue to be addressed. However, boron tends to have difficult in quantification with conventionally applied methods like EPMA and XPS. In this study, accelerator-driven neutron-imaging system was applied. Since boron is the material for neutron absorption, its sensitivity in terms of neutron penetration through specimens is concerned. To adjust neutron attenuation of a specimen to suit a particular measurement by selecting the neutron energy range, we focused on the energy resolved neutron imaging system RADEN, which utilizes wide energy range from meV to keV. Development of a method to visualize boron distribution using energy-resolved neutrons has been started. In this presentation the authors show the status of the development of a method utilizing energy-resolved neutrons and provide some outcome from its application to the Core Material Melting and Relocation (CMMR)-0 and -2 specimens.
Su, Y. H.; 及川 健一; 篠原 武尚; 甲斐 哲也; 堀野 孝*; 井戸原 修*; 三阪 佳孝*; 友田 陽*
Scientific Reports (Internet), 11, p.4155_1 - 4155_14, 2021/02
被引用回数：9 パーセンタイル：71.69(Multidisciplinary Sciences)A time-of-flight Bragg-edge neutron transmission imaging was used to investigate the microstructure and strain distributions in a gear hardened by a newly developed two-step induction-heating method: precursor (Sample 1) and final product (Sample 2). The edge- position and edge-broadening were determined and mapped with high spatial resolution, which enabled us to confirm the two-dimensional distributions of the microstructure and residual strain. A deep hardened layer was made for Sample 1 in which martensite was formed on the entire teeth and the outer peripheral portion of the gear body. Sample 2 was subjected to double induction-hardening, where a tempered martensite was formed as the thermal refined microstructure between a fine-grained martensite at the tooth surface and a ferrite-pearlite microstructure at the core. The relationship between edge-broadening and the Vickers hardness described by a linear equation was employed to derive the elastic residual strain. The residual strain map for Sample 2 revealed that a steep compressive strain was introduced into the fine-grained martensite at the tooth surface by the super rapid induction- heating and quenching process. The reversal of tension was speculated to occur below 2 mm from the tooth tip, and the strain was almost zero in the core region.
He neutron spin filter at J-PARC奥平 琢也; 奥 隆之; 猪野 隆*; 林田 洋寿*; 吉良 弘*; 酒井 健二; 廣井 孝介; 高橋 慎吾*; 相澤 一也; 遠藤 仁*; et al.
Nuclear Instruments and Methods in Physics Research A, 977, p.164301_1 - 164301_8, 2020/10
被引用回数：8 パーセンタイル：83(Instruments & Instrumentation)We are developing a neutron polarizer with polarized He gas, referred to as a He spin filter, based on the Spin Exchange Optical Pumping (SEOP) for polarized neutron scattering experiments at Materials and Life Science Experimental Facility (MLF) of Japan Proton Accelerator Research Complex (J-PARC). A He gas-filling station was constructed at J-PARC, and several He cells with long spin relaxation times have been fabricated using the gas-filling station. A laboratory has been prepared in the MLF beam hall for polarizing He cells, and compact pumping systems with laser powers of 30 W and 110 W, which can be installed onto a neutron beamline, have been developed. A He polarization of 85% was achieved at a neutron beamline by using the pumping system with the 110 W laser. Recently, the first user experiment utilizing the He spin filter was conducted, and there have been several more since then. The development and utilization of He spin filters at MLF of J-PARC are reported.
阿部 雄太; 土川 雄介; 甲斐 哲也; 松本 吉弘*; Parker, J. D.*; 篠原 武尚; 大石 佑治*; 加美山 隆*; 永江 勇二; 佐藤 一憲
Proceedings of 2020 International Conference on Nuclear Engineering (ICONE 2020) (Internet), 6 Pages, 2020/08
Boron carbide is used as a neutron-absorbing material in Fukushima-Daiichi Nuclear Power Station (1F), producing borides that are twice as hard as oxides (such as UO and ZrO). The high neutron absorption of boron affects the evaluation of re-criticality during the process of debris retrieval. Therefore, it is important not only to determine the presence of boron but also to investigate the distribution of boron inside the material in a non-destructive manner during decommissioning. To address the uncertainties in the core material relocation behavior of boiling water reactor (BWR) during a severe accident (SA), solidified melt specimens of a simulated fuel assembly were prepared by plasma heating. If core material melting and relocation (CMMR) specimens can be used to estimate the B distribution in 1F Unit-3, that will provide valuable information in the decommissioning of 1F. To address this, the authors focused on the energy-resolved neutron imaging system, RADEN, which utilizes a wide energy range, from meV to keV. This is an innovative three-dimensional analysis technology for boride distribution that affects the evaluation of hardness and re-criticality. In the calibration standard samples (Zr
B
and FeB), there was a good correlation between boron concentration and the energy-dependence of the cross sections of cold and epi-thermal neutrons. In the CMMR specimens, boron distribution was confirmed from the contrast difference between cold and epi-thermal neutrons. In the future, the results of calibration standard samples will be applied to the results of CMMR specimens. With this method, three-dimensional boron distribution will be measured, and the understanding of boride distribution 1F Unit-3 will be improved, which may be reflected in an improved SA code.
FeO
Cl with tunable direction in three dimensions阿部 伸行*; 塩澤 俊介*; 松浦 慧介*; 佐賀山 基*; 中尾 朗子*; 大原 高志; 徳永 祐介*; 有馬 孝尚*
Physical Review B, 101(18), p.180407_1 - 180407_5, 2020/05
被引用回数：2 パーセンタイル：18.66(Materials Science, Multidisciplinary)The correlation between magnetism and electric polarization in a chiral insulating magnet BaFeOCl has been investigated. The temperature dependence of magnetic susceptibility shows an anomaly at 564 K, suggesting the onset of antiferromagnetic order of Fe
moments. Electric polarization appears in a magnetic field below TN due to the spin-direction-dependent metal-ligand hybridization. The direction of the electric polarization can be controlled in three-dimensional space by changing the direction of an external magnetic field. This compound also shows an antiferromagnetic-to-weak-ferromagnetic transition accompanied by a structural phase transition at 140 K.
篠原 武尚; 甲斐 哲也; 及川 健一; 中谷 健; 瀬川 麻里子; 廣井 孝介; Su, Y. H.; 大井 元貴; 原田 正英; 飯倉 寛; et al.
Review of Scientific Instruments, 91(4), p.043302_1 - 043302_20, 2020/04
被引用回数：32 パーセンタイル：95.58(Instruments & Instrumentation)The energy-resolved neutron imaging system, RADEN, has been installed at the pulsed neutron source in the Materials and Life Science Experimental Facility of the Japan Proton Accelerator Research Complex. In addition to conventional neutron radiography and tomography, RADEN, the world's first imaging beam-line at a pulsed neutron source, provides three main options for new, quantitative neutron imaging techniques: Bragg-edge imaging to visualize the spatial distribution of crystallographic information, resonance absorption imaging for elemental composition and temperature information, and polarized neutron imaging for magnetic field information. This paper describes the results of characterization studies of the neutronic performance and installed devices at RADEN and shows the results of several demonstration studies for pulsed neutron imaging.
