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論文

Multiple metamagnetic transitions in the helical antiferromagnet CeVGe$$_{3}$$

Jin, H.*; Choi, E. S.*; Wu, H.-C.*; Curro, N. J.*; 那波 和宏*; 佐藤 卓*; 鬼柳 亮嗣; 大原 高志; Klavins, P.*; Taufour, V.*

Physical Review B, 111(3), p.035103_1 - 035103_7, 2025/01

 被引用回数:0 パーセンタイル:0.00(Materials Science, Multidisciplinary)

We report on neutron diffraction, magnetoresistance, magnetization and magnetic torque measurements under high magnetic field in the helical antiferromagnet CeVGe$$_{3}$$. This compound exhibits Kondo lattice coherence and helical antiferromagnetic (AFM) ordering at ambient pressure, similar to the well-studied CeRhIn$$_{5}$$. Our measurements reveal that CeVGe$$_{3}$$ undergoes a magnetic transition from an incommensurate (ICM) AFM state to an up-up-down-down commensurate (CM) AFM structure, followed by a transition to a novel phase at higher fields. A quantum phase transition occurs around 21.3 T. This rich magnetic field phase diagram closely resembles that of CeRhIn$$_{5}$$. Furthermore, angle-dependent magnetoresistance measurements reveal that all transitions in CeVGe$$_{3}$$ occur from the field component along the ab plane. These findings highlight the intricate interplay among exchange interactions, crystal field effects, ground state properties, and crystalline symmetries.

論文

Development of an Fe$$^{rm II}$$ complex exhibiting intermolecular proton shifting coupled spin transition

Ji, T.*; Su, S.*; Wu, S.*; 堀 優太*; 重田 育照*; Huang, Y.*; Zheng, W.*; Xu, W.*; Zhang, X.*; 鬼柳 亮嗣; et al.

Angewandte Chemie; International Edition, 63(25), p.e202404843_1 - e202404843_6, 2024/04

 被引用回数:0 パーセンタイル:0.00(Chemistry, Multidisciplinary)

In this study, we investigated reversible intermolecular proton shifting (IPS) coupled with spin transition (ST) in a novel Fe$$^{rm II}$$ complex. The host Fe$$^{rm II}$$ complex and the guest carboxylic acid anion were connected by intermolecular hydrogen bonds (IHBs). We extended the intramolecular proton transfer coupled ST phenomenon to the intermolecular system. The dynamic phenomenon was confirmed by variable-temperature single-crystal X-ray diffraction, neutron crystallography, and infrared spectroscopy.

論文

Quantum critical behavior of the hyperkagome magnet Mn$$_3$$CoSi

山内 宏樹; Sari, D. P.*; 安井 幸夫*; 坂倉 輝俊*; 木村 宏之*; 中尾 朗子*; 大原 高志; 本田 孝志*; 樹神 克明; 井川 直樹; et al.

Physical Review Research (Internet), 6(1), p.013144_1 - 013144_9, 2024/02

$$beta$$-Mn-type family alloys Mn$$_3$$$$TX$$ have three-dimensional antiferromagnetic (AFM) corner-shared triangular network. The antiferromagnet Mn$$_3$$RhSi shows magnetic short-range order (SRO) over a wide temperature range of approximately 500 K above the N$'{e}$el temperature $$T_{rm N}$$ = 190 K. Mn$$_3$$CoSi has the smallest lattice parameter and the lowest $$T_{rm N}$$ in the family compounds. The quantum critical point (QCP) from AFM to the quantum paramagnetic state is expected near a cubic lattice parameter of 6.15 $AA. Although $T_N$$ of Mn$$_3$$CoSi is only 140 K, quantum critical behavior is observed in Mn$$_3$$CoSi as the enhancement of the electronic specific heat coefficient $$gamma$$. We study how the magnetic SRO appears in Mn$$_3$$CoSi by using neutron scattering, $$mu$$SR, and physical property measurements. The experimental results show that the neutron scattering intensity of the magnetic SRO does not change much regardless of the suppressed magnetic moment in the long-range magnetic ordered state compared to those of Mn$$_3$$RhSi. The initial asymmetry drop ratio of $$mu$$SR above $$T_{rm N}$$ becomes small, and the magnetic SRO temperature $$T_{SRO}$$ is suppressed to 240 K. The results suggest that the Mn$$_3$$CoSi is close to the QCP in the Mn$$_3$$$$TX$$ system.

論文

Chiral Dirac fermion in a collinear antiferromagnet

Zhang, A.*; Deng, K.*; Sheng, J.*; Liu, P.*; Kumar, S.*; 島田 賢也*; Jiang, Z.*; Liu, Z.*; Shen, D.*; Li, J.*; et al.

Chinese Physics Letters, 40(12), p.126101_1 - 126101_8, 2023/12

 被引用回数:11 パーセンタイル:83.08(Physics, Multidisciplinary)

In a Dirac semimetal, the massless Dirac fermion has zero chirality, leading to surface states connected adiabatically to a topologically trivial surface state as well as vanishing anomalous Hall effect. Recently, itis predicted that in the nonrelativistic limit of certain collinear antiferromagnets, there exists a type of chiral "Dirac-like" fermion, whose dispersion manifests four-fold degenerate crossing points formed by spin-degenerate linear bands, with topologically protected Fermi arcs. Here, by combining with neutron diffraction and first-principles calculations, we suggest a multidomain collinear antiferromagnetic configuration, rendering the existence of the Fermi-arc surface states induced by chiral Dirac-like fermions.

論文

The Hydrogen-bond network in sodium chloride tridecahydrate; Analogy with ice VI

山下 恵史朗*; 中山 和也*; 小松 一生*; 大原 高志; 宗像 孝司*; 服部 高典; 佐野 亜沙美; 鍵 裕之*

Acta Crystallographica Section B; Structural Science, Crystal Engineering and Materials (Internet), 79(5), p.414 - 426, 2023/10

 被引用回数:2 パーセンタイル:43.78(Chemistry, Multidisciplinary)

最近発見された塩化ナトリウムの超水和物(NaCl$$cdot$$ 13H(D)$$_{2}$$O)の構造を1.7GPa, 298Kでのその場単結晶中性子回折によって決定した。この物質は大きな水素結合ネットワークを持ち、いくつかの水分子は分岐水素結合や5配位水分子のような歪んだ結合の特徴を持つ。水素結合ネットワークは、ネットワークトポロジーと水素結合の無秩序性という点で、氷VIと類似している。擬似対称性によって接続されたネットワークの構成要素を区別しなければ、このハイドレートの全体的なネットワーク構造は、氷VIのネットワーク構造に対応する小さな構造単位に分解することで表現できる。この水素結合ネットワークは、既知の塩水和物とは対照的に、水分子の配向の乱れを含んでいる。ここでは、イオン種を含む水素結合ネットワークに関するさらなる洞察のための例を示す。

論文

Site-specific relaxation of peptide bond planarity induced by electrically attracted proton/deuteron observed by neutron crystallography

千葉 薫*; 松井 拓郎*; 茶竹 俊行*; 大原 高志; 田中 伊知朗*; 油谷 克英*; 新村 信雄*

Protein Science, 32(10), p.e4765_1 - e4765_13, 2023/10

 被引用回数:0 パーセンタイル:0.00(Biochemistry & Molecular Biology)

In structural biology, peptide bonds, fundamental linkages between hundreds of amino acids, of which a protein molecule is composed, have been commonly treated as a plane structure just as Linus Pauling et al. proposed. In this paper, a site-specific peptide bond relaxation mechanism by deuterons whose localization has been suggested by neutron crystallography is proposed. A comprehensive study using X-ray and neutron diffraction and $$^{15}$$N chemical shifts of individual amide nitrogen atoms within the same peptide bond strongly suggests the relaxation of the electronic resonance structure because of site-specific modulation by protons/deuterons localized on the electron orbital of the carbonyl oxygen.

論文

Development of an iron(II) complex exhibiting thermal- and photoinduced double proton-transfer-coupled spin transition in a short hydrogen bond

中西 匠*; 堀 優太*; 重田 育照*; 佐藤 寛泰*; 鬼柳 亮嗣; 宗像 孝司*; 大原 高志; 岡澤 厚*; 島田 林太郎*; 坂本 章*; et al.

Journal of the American Chemical Society, 145(35), p.19177 - 19181, 2023/08

 被引用回数:5 パーセンタイル:51.73(Chemistry, Multidisciplinary)

Multiple proton transfer (PT) controllable by external stimuli plays a crucial role in fundamental chemistry, biological activity, and material science. However, in crystalline systems, controlling multiple PT, which results in a distinct protonation state, remains challenging. In this study, we developed a novel tridentate ligand and iron(II) complex with a short hydrogen bond (HB) that exhibits a PT-coupled spin transition (PCST). Single-crystal X-ray and neutron diffraction measurements revealed that the positions of the two protons in the complex can be controlled by temperature and photoirradiation based on the thermal- and photoinduced PCST. The obtained results suggest that designing molecules that form short HBs is a promising approach for developing multiple PT systems in crystals.

論文

Magnetic ordering and structural phase transitions of Nd$$_{3}$$$$T$$$$_{4}$$Sn$$_{13}$$ ($$T$$ = Rh and Ir)

下田 愛海*; 岩佐 和晃*; 桑原 慶太郎*; 佐賀山 基*; 中尾 裕則*; 石角 元志*; 大原 高志; 中尾 朗子*; 星川 晃範*; 石垣 徹*

JPS Conference Proceedings (Internet), 38, p.011091_1 - 011091_6, 2023/05

Synchrotron X-ray diffraction study revealed that Nd$$_{3}$$$$T$$$$_{4}$$Sn$$_{13}$$ ($$T$$ = Rh and Ir) undergo structural phase transitions characterized by the wave vector $$q$$$$_{rm L}$$=(1/2,1/2,0). Neutron diffraction study revealed antiferromagnetic ordering below $$T$$$$_{rm N}$$ = 1.65 and 1.42 K for Nd$$_{3}$$Rh$$_{4}$$Sn$$_{13}$$ and Nd$$_{3}$$Ir$$_{4}$$Sn$$_{13}$$, respectively, which is similar to that previously reported for Nd$$_{3}$$Co$$_{4}$$Sn$$_{13}$$. These compounds show a magnetic susceptibility saturation behavior below approximately 3 K. The results indicate emergence of anomalous electronic correlation in Nd$$_{3}$$$$T$$$$_{4}$$Sn$$_{13}$$ ($$T$$ = Co, Rh, and Ir) above $$T$$$$_{rm N}$$.

論文

Observation of proton-transfer-coupled spin transition by single-crystal neutron-diffraction measurement

中西 匠*; 堀 優太*; 重田 育照*; 佐藤 寛泰*; Wu, S.-Q.*; 鬼柳 亮嗣; 宗像 孝司*; 大原 高志; 佐藤 治*

Physical Chemistry Chemical Physics, 25(17), p.12394 - 12400, 2023/05

 被引用回数:3 パーセンタイル:42.17(Chemistry, Physical)

The application of single-crystal neutron diffraction (SCND) to observe proton-transfer phenomena in crystalline compounds exhibiting unusual protonation states or proton dynamics has garnered significant research interest in recent years. However, proton tautomerism, which results in different protonation states before and after proton transfer, has never been observed using the SCND technique. Thus, to observe the proton tautomerism phenomenon by SCND measurements, we developed an iron(II) complex that forms a large crystal and exhibits a proton-transfer-coupled spin transition (PCST). The presence of the two types of proton tautomers was determined by conventional analysis of the proton position by X-ray crystallography, infrared spectroscopy, and density functional theory calculations. Finally, our results confirmed that proton tautomerism was successfully observed for the first time using variable-temperature SCND measurements.

論文

Solid-state far-ultraviolet C light sources for the disinfection of pathogenic microorganisms using graphene nanostructure field emitters

根尾 陽一郎*; 橋本 凱*; Koike, Rei*; 大原 高志; 松本 貴裕*

Global Challenges, 7(4), p.2200236_1 - 2200236_8, 2023/04

 被引用回数:1 パーセンタイル:13.37(Multidisciplinary Sciences)

The ongoing global outbreak of coronavirus disease has necessitated the use of ultraviolet (UV) disinfection techniques to reduce viral transmission in public places. The previously used UV wavelength is harmful to the human body, the wavelength range from 200 to 235 nm, often referred to as far-UVC light, has attracted attention as a novel disinfection wavelength range that can be used in a safe manner. Here, an efficient mercury-free far-UVC solid-state light source is presented. This light source demonstrates intense 230 nm emission with a narrow spectral width of 30 nm and a long lifetime of more than 1000 h. These characteristics can be achieved by graphene nanostructure field emitters and wide-bandgap magnesium aluminate phosphors.

論文

Hybridization of wide-angle X-ray and neutron diffraction techniques in the crystal structure analyses of synthetic polymers

田代 孝二*; 日下 勝弘*; 山元 博子*; 細谷 孝明*; 岡田 修司*; 大原 高志

Polymers (Internet), 15(2), p.465_1 - 465_44, 2023/01

 被引用回数:3 パーセンタイル:11.04(Polymer Science)

The development in the crystal structure analysis of synthetic polymers using the hybridized combination of wide-angle X-ray and neutron diffraction (WAXD and WAND, respectively) techniques has been reviewed with many case studies performed by the authors. At first, the technical development was reviewed. Secondly, the usage of the WAND method was introduced, in which the successful extraction of hydrogen atomic positions was described. The third example is to show the importance for the hybrid combination of these two diffraction methods. Finally, the application of WAND technique in the trace of structural changes induced under the application of external stress or temperature was described. The future perspective is described for the development of structural science of synthetic polymers on the basis of the combined WAXD/WAND techniques.

論文

Rearrangement of hydrogen bonds in dehydrated raffinose tetrahydrate; A Time-of-flight neutron diffraction study

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:0.00(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 ${it moderate}$ O-H...O hydrogen bonds and ${it weak}$ 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.

論文

Evaluation of detector performances of new thin position-sensitive scintillation detectors for SENJU diffractometer

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 2022 IEEE Nuclear Science Symposium, Medical Imaging Conference and Room Temperature Semiconductor Detector Conference (2022 IEEE NSS MIC RTSD) (Internet), 2 Pages, 2022/11

J-PARC物質・生命科学実験施設に設置されたSENJU回折計用として、新たに薄型の位置敏感シンチレータ中性子検出器を開発した。本検出器は既設のオリジナル検出器と同等の有感面積(256$$times$$256mm)とピクセル分解能(4$$times$$4mm)を保持しつつ、奥行きは12cm(オリジナルの40%)の薄型へと改良した。製作した6台の検出器はいずれも検出効率60%(2A)、計数均一性5-8%と良好な性能を示した。現在、これらの検出器はビームライン内の回折計に装填されており、数か月の安定動作が確認されている。

論文

単結晶中性子回折法の開発と高精度な水素原子位置の決定に基づいた構造化学研究

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。

論文

Single-crystal structure analysis of non-deuterated triglycine sulfate by neutron diffraction at 20 and 298 K; A New disorder model for the 298 K structure

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.

論文

Improvement of nano-polycrystalline diamond anvil cells with Zr-based bulk metallic glass cylinder for higher pressures; Application to Laue-TOF diffractometer

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:4 パーセンタイル:47.58(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$$_{4}$$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.

論文

Insights into proton dynamics in a photofunctional salt-cocrystal continuum; Single-crystal X-ray, neutron diffraction, and Hirshfeld atom refinement

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:11 パーセンタイル:48.69(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.

論文

Two-dimensional scintillation neutron detectors for the extension of SENJU diffractometer

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$$times$$256mm)とピクセル分解能(4$$times$$4mm)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${AA}$)、$$^{60}$$Coガンマ感度1$$times$$10$$^{-5}$$、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。

論文

Charge-density-wave order and multiple magnetic transitions in divalent europium compound EuAl$$_4$$

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:52 パーセンタイル:95.02(Physics, Multidisciplinary)

Multiple transition phenomena in divalent Eu compound EuAl$$_4$$ 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 $$q_{rm CDW}$$ = (0 0 $${delta}_c$$). In contrast, magnetic peaks appear at $$q_2 = ({delta}_2 {delta}_2 0)$$ with $${delta}_2$$ = 0.09 below $$T_{N1}$$ = 15.4 K, and moves to $$q_1 = ({delta}_1 0 0)$$ with $${delta}_1$$ = 0.19 below $$T_{N3}$$ =12.2 K, whereas no distinct change in the magnetic Bragg peak was detected at $$T_{N2}$$ and $$T_{N4}$$. The structural modification with $$q_{rm CDW}$$ is characterized by an absence of the superlattice peak in (0 0 $$l$$). Considering an absence of splitting in magnetic peaks along $$l$$, the structural transition is mainly ascribed to a displacement of Al ions within the tetragonal $$ab$$-plane. Complex incommensurate magnetic transitions are in stark contrast to a simple collinear commensurate structure in isovalent EuGa$$_4$$. This could stem from incompatible electronic structures with the CDW transition between two compounds.

論文

Quantum proton entanglement on a nanocrystalline silicon surface

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:1 パーセンタイル:4.81(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.

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