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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

https://doi.org/10.1088/0256-307X/40/12/126101

被引用回数：1 パーセンタイル：0(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

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

https://doi.org/10.1021/jacs.3c06323

被引用回数：0 パーセンタイル：0(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 $_{3}$ $_{4}$ Sn $_{13}$ ( = 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

https://doi.org/10.7566/JPSCP.38.011091

Synchrotron X-ray diffraction study revealed that Nd $_{3}$ $_{4}$ Sn $_{13}$ ( = Rh and Ir) undergo structural phase transitions characterized by the wave vector $_{rm L}$ =(1/2,1/2,0). Neutron diffraction study revealed antiferromagnetic ordering below $_{rm N}$ = 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 $_{3}$ $_{4}$ Sn $_{13}$ ( = Co, Rh, and Ir) above $_{rm N}$ .

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

https://doi.org/10.1039/D3CP00527E

被引用回数：1 パーセンタイル：56.86(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

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

https://doi.org/10.1107/S2056989022000858

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

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

https://doi.org/10.1002/chem.202103044

被引用回数：4 パーセンタイル：30.82(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

https://doi.org/10.1109/NSS/MIC42677.2020.9507813

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(256256mm)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)、 $^{60}$ Coガンマ感度110 $^{-5}$ 、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

Programmable synthesis of silver wheels

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

https://doi.org/10.1021/acs.inorgchem.1c00106

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 $^{rm H2O}$ 5Ag $^{rm OH}$ 4Ag $^{rm OH}$ . The central hydroxides in 4Ag $^{rm OH}$ and 5Ag $^{rm OH}$ 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.

論文

Correlated Li-ion migration in the superionic conductor Li $_{10}$ GeP $_{2}$ S $_{12}$

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

https://doi.org/10.1039/D1TA00552A

被引用回数：19 パーセンタイル：80.41(Chemistry, Physical)

Herein, we studied the crystalline compound Li $_{10}$ GeP $_{2}$ S $_{12}$ 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.

論文

Magnetically induced electric polarization in Ba $_{3}$ Fe $_{2}$ O $_{5}$ Cl $_{2}$ 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

https://doi.org/10.1103/PhysRevB.101.180407

被引用回数：2 パーセンタイル：12.9(Materials Science, Multidisciplinary)

The correlation between magnetism and electric polarization in a chiral insulating magnet Ba $_{3}$ Fe $_{2}$ O $_{5}$ Cl $_{2}$ has been investigated. The temperature dependence of magnetic susceptibility shows an anomaly at 564 K, suggesting the onset of antiferromagnetic order of Fe $^{3+}$ 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.

論文

Successive phase transitions in $R_{3}$ Ir $_{4}$ Sn $_{13}$ (: La and Ce) investigated using neutron and X-ray diffraction

中里晟也*; 岩佐和晃*; 橋本大輔*; 塩澤真未*; 桑原慶太郎*; 中尾裕則*; 佐賀山基*; 石角元志*; 大原高志; 中尾朗子*; et al.

JPS Conference Proceedings (Internet), 30, p.011128_1 - 011128_6, 2020/03

https://doi.org/10.7566/JPSCP.30.011128

Successive phase transitions of $R_{3}$ Ir $_{4}$ Sn $_{13}$ (: La and Ce) were studied using neutron and X-ray diffraction techniques. A semimetal Ce $_{3}$ Ir $_{4}$ Sn $_{13}$ undergoes three phase transitions: an antiferromagnetic ordering characterized by a propagation vector $q_{rm M}$ = (1/2, 1/2, 2/5) below 0.6 K, a structural transformation with $q_{rm S2}$ = (1/4, 1/4, 1/4) at 2.0 K, and another structural transformation with $q_{rm S1}$ = (1/2, 1/2, 0) above room temperature. La $_{3}$ Ir $_{4}$ Sn $_{13}$ was confirmed to be a superconductor below 2.5 K under the $q_{rm S1}$ = (1/2, 1/2, 0) structure that also appears above room temperature.

論文

Crystal structure and cation distribution of the X-type hexaferrite Sr $_{2}$ Co $_{2}$ Fe $_{28}$ O $_{46}$

駒淵舞*; 漆原大典*; 浅香透*; 福田功一郎*; 大原高志; 宗像孝司*; 石川喜久*

Journal of the Physical Society of Japan, 89(3), p.034601_1 - 034601_5, 2020/03

https://doi.org/10.7566/JPSJ.89.034601

被引用回数：2 パーセンタイル：22.16(Physics, Multidisciplinary)

The crystal structure of an X-type hexaferrite Sr $_{2}$ Co $_{2}$ Fe $_{28}$ O $_{46}$ was investigated by the X-ray and neutron diffraction methods for a single crystal. Sr $_{2}$ Co $_{2}$ Fe $_{28}$ O $_{46}$ has the crystal structure described as a space group () and its lattice constants are = 5.9165(2) ; and = 84.1395(33) ; at 843 K. Co ions are almost localized in the octahedral site () in the middle of S $^{*}$ S $^{*}$ blocks. In addition, the adjacent octahedral and tetrahedral sites to site contain the significant number of Co $^{2+}$ .

論文

Magnetic, thermal, and neutron diffraction studies of a coordination polymer; bis(glycolato)cobalt(II)

中根僚宏*; 米山翔太*; 兒玉健*; 菊地耕一*; 中尾朗子*; 大原高志; 東中隆二*; 松田達磨*; 青木勇二*; 藤田渉*

Dalton Transactions (Internet), 48(1), p.333 - 338, 2019/01

https://doi.org/10.1039/C8DT04358B

被引用回数：2 パーセンタイル：11.34(Chemistry, Inorganic & Nuclear)

The two-dimensional quadratic lattice magnet, bis(glycolato)cobalt(II) ([Co(HOCH $_{2}$ CO $_{2}$ ) $_{2}$ ]), showed anti-ferromagnetic ordering at 15.0 K and an abrupt increase in magnetisation at H = 22 600 Oe and 2 K, thereby acting as a metamagnet. Neutron diffraction studies suggested that the magnetic moment vectors of the Co(II) ions had an amplitude of 3.59 mB and were not aligned in a fully antiparallel fashion to those of their neighbours, which caused canting between the magnetic moment vectors in the sheet. The canting angle was determined to be 7.1deg. Canting induced net magnetisation in the sheet, but this magnetisation was cancelled between sheets. The magnetisations in the sheets were oriented parallel to the magnetic field at the critical magnetic field.

論文

High oxide-ion conductivity in Si-deficient La $_{9.565}$ (Si $_{5.826}$ [] $_{0.174}$ )O $_{26}$ apatite without interstitial oxygens due to the overbonded channel oxygens

藤井孝太郎*; 八島正知*; 日比野圭祐*; 白岩大裕*; 福田功一郎*; 中山享*; 石沢伸夫*; 花島隆泰*; 大原高志

Journal of Materials Chemistry A, 6(23), p.10835 - 10846, 2018/06

https://doi.org/10.1039/C8TA02237B

被引用回数：27 パーセンタイル：70.21(Chemistry, Physical)

Apatite-type rare earth silicates are attractive materials with exhaust application such as solid-oxide fuel cells, due to its extremely high oxide-ion conductivity below 600 $^{circ}$ C. Interstitial (excess) oxygens have been believed to be responsible for the high conductivity in apatite-type materials. On the contrary, the present study clearly reveals the presence of Si vacancies [] in La-rich La $_{9.565}$ (Si $_{5.826}$ []] $_{0.174}$ )O $_{26}$ instead of the interstitial oxygens, by single-crystal neutron and X-ray diffraction analyses, density measurements and electronic calculations.

論文

Magnetic-ordering propagation vectors of terbium hexaboride revisited

岩佐和晃*; 伊賀文俊*; 茂吉武人*; 中尾朗子*; 大原高志

Journal of the Physical Society of Japan, 87(6), p.064705_1 - 064705_5, 2018/06

https://doi.org/10.7566/JPSJ.87.064705

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

The magnetic-ordered state of a single-crystal sample of TbB $_{6}$ has been studied with the high-precision neutron diffraction instrument SENJU installed at BL18 of the Materials and Life Science Facility in J-PARC. We observed new Bragg-reflection spots characterized by a propagation vector $q_{rm M2}$ = (1/4, 1/4, 0) below the Nel temperature $T_{rm N}$ 20 K, in addition to the $q_{rm M1}$ = (1/4, 1/4. 1/2) reported in the previous literatures. Because X-ray Thomson scattering measurements do not detect the $q_{rm M2}$ superlattice reflections at 13 K, $q_{rm M2}$ is a new magnetic-ordering propagation vector. The magnetic multi-q structure of TbB $_{6}$ is similar to that of CeB $_{6}$ , whereas the ratio of the $q_{rm M2}$ amplitude to that of qM1 is smaller than in CeB $_{6}$ . The combination of $q_{rm M1}$ and $q_{rm M2}$ is expected to assist the $q_{rm L1}$ = (1/2, 0, 0) lattice modulation.

論文

Non-aqueous selective synthesis of orthosilicic acid and its oligomers

五十嵐正安*; 松本朋浩*; 八木橋不二夫*; 山下浩*; 大原高志; 花島隆泰*; 中尾朗子*; 茂吉武人*; 佐藤一彦*; 島田茂*

Nature Communications (Internet), 8, p.140_1 - 140_8, 2017/07

https://doi.org/10.1038/s41467-017-00168-5

被引用回数：25 パーセンタイル：64.07(Multidisciplinary Sciences)

Orthosilicic acid (Si(OH) $_{4}$ ) and its small condensation compounds are among the most important silicon compounds but have never been isolated, despite the long history of intense research due to their instability. These compounds would be highly useful building blocks for advanced materials if they become available at high purity. We developed a simple procedure to selectively synthesize orthosilicic acid, its dimer, cyclic trimer, and tetramer, as well as appropriate conditions to stabilize these species, in organic solvents. Isolation of orthosilicic acid, the dimer and the cyclic tetramer as hydrogen-bonded crystals with tetrabutylammonium halides and of the cyclic trimer as solvent-containing crystals was achieved. The solid-state structures of these compounds were unambiguously clarified by single crystal X-ray diffraction analysis and also by neutron diffraction study for orthosilicic acid. Based on these results, we also succeeded in developing a more practical synthetic procedure for high concentrations of stable orthosilicic acid stably in organic solvents via a simple hydrolysis of tetraalkoxysilanes.

論文

Molecular gyrotops with a five-membered heteroaromatic ring; Synthesis, temperature-dependent orientation of dipolar rotors inside the crystal, and its birefringence change

増田敏幸*; Arase, Junko*; 稲垣佑亮*; 川幡正俊*; 山口健太郎*; 大原高志; 中尾朗子*; 門馬洋行*; Kwon, E.*; 瀬高渉*

Crystal Growth & Design, 16(8), p.4392 - 4401, 2016/08

https://doi.org/10.1021/acs.cgd.6b00508

被引用回数：27 パーセンタイル：87.56(Chemistry, Multidisciplinary)

Three-dimensional arrays of dipolar rotors were constructed as single crystals of molecular gyrotops, which are macrocage molecules with a bridged dipolar rotor. In this study, we synthesized novel molecular gyrotops with a five-membered heteroring, i.e., furan-diyl, thiophenediyl, and selenophene-diyl, and investigated the temperature-dependent orientation and rotation of the dipolar rotors inside the crystal.

論文

SENJU; A New time-of-flight single-crystal neutron diffractometer at J-PARC

大原高志; 鬼柳亮嗣; 及川健一; 金子耕士; 川崎卓郎; 田村格良; 中尾朗子*; 花島隆泰*; 宗像孝司*; 茂吉武人*; et al.

Journal of Applied Crystallography, 49(1), p.120 - 127, 2016/02

https://doi.org/10.1107/S1600576715022943

被引用回数：51 パーセンタイル：95.86(Chemistry, Multidisciplinary)

SENJU, a time-of-flight Laue-type single-crystal neutron diffractometer, was developed at the Materials and Life Science Experimental Facility (MLF) of the Japan Accelerator Research Complex (J-PARC). Molecular structure analysis of a sub-millimeter taurine crystal and magnetic structure analysis of a MnF $_{2}$ crystal were performed to evaluate its performance.

論文

Single-crystal neutron diffraction study of the heavy-electron superconductor CeNiGe $_{3}$

池田陽一*; 植田大地*; 吉澤英樹*; 中尾朗子*; 宗像孝司*; 大原高志

Journal of the Physical Society of Japan, 84(12), p.123701_1 - 123701_5, 2015/12

https://doi.org/10.7566/JPSJ.84.123701

被引用回数：4 パーセンタイル：34.89(Physics, Multidisciplinary)

特異な反強磁性秩序化を示すことが知られているheavy-electron超伝導体であるCeNiGe $_{3}$ について、MLFのSENJUを用いて単結晶中性子回折測定を行った。相転移温度の5K以下で測定を行ったところ、以前の粉末試料を用いた回折測定では伝搬ベクトルとして $k_{1}$ =(1,0,0)と $k_{2}$ =(0,0.41,1/2)が観測されたのに対して、単結晶試料を用いた測定では $k_{2}$ =(0,0.41,1/2)のみが観測された。このことから、CeNiGe $_{3}$ の常圧における磁気特性は伝搬ベクトル $k_{2}$ のみによって特徴づけられることが示唆された。

論文

Proton order-disorder phenomena in a hydrogen-bonded rhodium- $^{5}$ -semiquinone complex; A Possible dielectric response mechanism

満身稔*; 江崎一成*; 小松裕貴*; 鳥海幸四郎*; 宮東達也*; 水野元裕*; 東信晃*; 宮崎裕司*; 中野元裕*; 北河康隆*; et al.

Chemistry; A European Journal, 21(27), p.9682 - 9696, 2015/06

https://doi.org/10.1002/chem.201500796

被引用回数：7 パーセンタイル：25.07(Chemistry, Multidisciplinary)

A newly synthesized one-dimensional (1D) hydrogen-bonded (H-bonded) rhodium(II)- $^{5}$ -semiquinone complex, [Cp $^{*}$ Rh( $^{5}$ --HSQ-Me $_{4}$ )]PF $_{6}$ exhibits a paraelectric-;antiferroelectric second-order phase transition at 237.1 K. Neutron and X-ray crystal structure analyses reveal that the H-bonded proton is disordered over two sites in the room-temperature (RT) phase. The phase transition would arise from this proton disorder together with rotation or libration of the Cp $^{*}$ ring and PF $_{6}$ ion. The relative permittivity $_{b}$ ' along the H-bonded chains reaches relatively high values (ca., 130) in the RT phase.