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Ba
(PO
) ( = Mg, Mn, Co, and Ni)梶田 遥一*; 永井 隆之*; 山岸 茂直*; 木村 健太*; 萩原 雅人; 木村 剛*
Chemistry of Materials, 36(15), p.7451 - 7458, 2024/08
Ferroaxial transitions of Na
Ba(PO
) ( = Mg, Mn, Co, and Ni) with the glaserite structure, featuring rotational distortions of PO tetrahedra, are investigated. Neutron powder diffraction (NPD) measurements on polycrystalline samples were carried out in the temperature range from room temperature to 800 K. Structure analyses on the NPD data revealed that all of the compounds studied here have a ferroaxial structure (space group: 
)at room temperature and undergo a ferroaxial transition into a non-ferroaxial phase (space group: 
1) upon heating. Structural parameters change continuously at the transition temperature, which suggests that the ferroaxial transition of NaBa(PO) systems is of the second order. Furthermore, to examine the structural stability, ab initio phonon calculations were carried out for NaBaMg(PO). The calculated result shows that the rotational phonon mode instability inherent in the non-ferroaxial 1 phase leads to the phases as a ground state, which well explains the experimental result. This study revealed that NaBa (PO) systems with the glaserite structure are a class of ferroaxial compounds showing a second-order pure ferroaxial transition.
永井 隆之*; 萩原 雅人; 横井 里江*; 森分 博紀*; 木村 剛*
Journal of the American Chemical Society, 146(33), p.23348 - 23355, 2024/08
Ferroelectric materials compatible with magnetism and/or conductive properties provide a platform for exploring unconventional phenomena, such as the magnetoelectric effect, nonreciprocal responses, and nontrivial superconductivity. Though recent studies on multiferroics have offered several approaches, the search for magnetic and/or conducting ferroelectric materials is still a challenging issue under the traditional "d
-ness" rule, refusing active d electrons. Here, we propose the emergence of ferroelectricity through a combination of crystallographic chirality and axial vector, accepting even non-d magnetic ions. This proposal is demonstrated in quasi-one-dimensional magnetic systems SrMVO
(M = Ni, Mg, and Co). The ferroelectric phase transition is observed by measurements of neutron powder diffraction and dielectric properties in all compositions. Structural analyses and first-principles calculations indicate that these magnetic compounds are identified as proper-type ferroelectrics whose ferroelectric phase transition is achieved by spiral motions of crystallographic screw chains formed by edge-shared MO6 octahedra, considered as the combination of locally defined chirality and axial vector. Computationally predicted magnitude of spontaneous polarization of SrMVO reaches 
10
C/cm
, comparable to that of conventional ferroelectrics, despite the incorporation of non-d magnetic elements. The mechanism proposed in this study offers a unique approach to the exploration of new ferroelectrics beyond the traditional paradigms.
金子 耕士; 田端 千紘; 萩原 雅人; 山内 宏樹; 大場 洋次郎; 熊田 高之; 久保田 正人; 児島 佑樹*; 生田目 望; 佐々木 未来; et al.
JPS Conference Proceedings (Internet), 41, p.011015_1 - 011015_6, 2024/03
We will introduce our recent update on low temperature system for neutron diffraction experiments. This is characterized by advantages such as liquid He free and sophisticated automatic temperature control functions, which can be a new standard for low temperature and high magnetic field experiments of neutron scattering.
平田 芳信*; 中川 洋; 山内 宏樹; 金子 耕士; 萩原 雅人; 山口 秀幸*; 大元 智絵*; 勝野 那嘉子*; 今泉 鉄平*; 西津 貴久*
Food Hydrocolloids, 141, p.108728_1 - 108728_7, 2023/08
被引用回数：2 パーセンタイル：66.25(Chemistry, Applied)結晶化度は食品や材料の機械的性質に反映される。結晶化度は澱粉の構造ダイナミクスと関係しているはずである。本研究では、中性子準弾性散乱(QENS)を用いて、炊飯澱粉の老化に伴う分子ダイナミクスの変化を調べた。測定されたQENSの幅は老化に伴い狭くなった。また、弾性非干渉散乱構造因子(EISF)は増加し、老化現象に伴い分子ダイナミクスが空間的に抑制されることが示された。低移動度と高移動度をそれぞれ結晶相と非晶質相に対応させた2値分布の連続拡散モデルを用いてEISFを解析したところ、低移動度成分の割合が老化によって増加することが示された。
金子 耕士; 田端 千紘; 萩原 雅人; 山内 宏樹; 久保田 正人; 長壁 豊隆; 大貫 惇睦*
Journal of the Physical Society of Japan, 92(8), p.085001_1 - 085001_2, 2023/08
被引用回数：0 パーセンタイル：0.00(Physics, Multidisciplinary)A magnetic order in orthorhombic GdCu was investigated by a single crystal neutron diffraction with thermal neutron. Magnetic peaks were observed at incommensurate positions described by the ordering vector 
=(
~1~0) with =0.678 at 4~K. This ordering vector is close to the commensurate one with 
=(2/3~1~0) reported earlier, but clearly deviates. The incommensurate nature of the magnetic order in GdCu is further corroborated by the peak shift with temperature below 
.
HO藤原 理賀; 萩原 雅人; 森田 克洋*; 村井 直樹; 幸田 章宏*; 岡部 博孝*; 満田 節生*
Physical Review B, 107(5), p.054435_1 - 054435_8, 2023/02
被引用回数：0 パーセンタイル：0.00(Materials Science, Multidisciplinary)
= 1/2ハイゼンベルグ直線鎖反強磁性体は、最も単純なスピンモデルであるが、様々な量子多体現象のプラットフォームを提供する。この論文では、準一次元反強磁性体KCuPOHOの磁性を報告した。
= 11.7(1) Kにおいて、格子整合な長距離反強磁性秩序が形成され、その磁気モーメントの大きさは0.31(1) 
である事がわかった。また鎖内相互作用
と鎖間相互作用
の大きさはそれぞれ172Kと4.25(4) Kと見積もられ、/の比は0.0247(3)である。中性子非弾性散乱実験により、より高温では、一次元ハイゼンベルグ量子スピン鎖の特徴である連続体励起スペクトルが観測され、より低温では、分散励起にスピンギャップが観測された。これらの結果は、弱く結合した = 1/2ハイゼンベルグスピン鎖系で観測される性質と一致する。
山岸 茂直*; 林田 健志*; 三澤 龍介*; 木村 健太*; 萩原 雅人; 村田 智城*; 廣瀬 左京*; 木村 剛*
Chemistry of Materials, 35(2), p.747 - 754, 2023/01
被引用回数：5 パーセンタイル：86.76(Chemistry, Physical)The so-called "ferroaxial transition" characterized by a rotational structural distortion that breaks a mirror symmetry has gained growing interest in terms of a new class of ferroic state in crystalline materials. RbFe(MoO) which belongs to glaserite-type compounds, X□;1 Y□;2 [M(TO
], is one of the most representative materials showing a ferroaxial transition, i.e., ferroaxial materials. Considering a variety of glaserite-type compounds, we expect that they provide a good arena for ferroaxial materials. In this work, we explored new ferroaxial materials by formula-based screening using regular expression search and symmetry detection algorithm. As a result, we found that a glaserite-type compound, KZr(PO), is one of the promising candidates for ferroaxial materials. Experimentally, we demonstrate that KZr(P O) shows a ferroaxial transition at about 700 K, which is well explained by ab initio phonon calculations. The ferroaxial nature of KZr(PO) is further confirmed by the observation of its domain structures using a linear electrogyration effect, that is, optical rotation in proportion to an applied electric field. Our work provides an effective approach to exploring ferroaxial materials.
Fe
GeO
with andalusite structure柿本 和勇*; 高田 早紀*; 太田 寛人*; 原口 祐哉*; 萩原 雅人; 鳥居 周輝*; 神山 崇*; 三田村 裕幸*; 徳永 将史*; 畠山 温*; et al.
Journal of the Physical Society of Japan, 91(5), p.054704_1 - 054704_7, 2022/05
被引用回数：1 パーセンタイル：24.98(Physics, Multidisciplinary)The magnetism of AlFeGeO from 
to 
with the andalusite structure was examined. AlFeGeO at low temperatures was found to show a weak ferromagnet-like behavior for 
and a spin glass behavior for 
. The small spontaneous magnetization observed in the weak ferromagnet-like samples may be caused by the existence of Dzyaloshinsky-Moriya interaction and the difference in the magnitude of the magnetic moments of Fe
in the octahedral and trigonal bipyramidal sites. The appearance of the spin glass behavior implies that the dilution of Fe ions by Al ions in AlFeGeO causes the competition between ferromagnetic and antiferromagnetic interactions. The 
dependence of the site occupancy of Fe ions suggests that FeGeO with the andalusite structure cannot be synthesized.
-xGeO with = 0.09 and 0.15柿本 和勇*; 太田 寛人*; 原口 祐哉*; 萩原 雅人; 鳥居 周輝*; 神山 崇*; 香取 浩子*
Journal of the Physical Society of Japan, 91(5), p.054707_1 - 054707_9, 2022/05
被引用回数：0 パーセンタイル：0.00(Physics, Multidisciplinary)Neutron diffraction experiments on polycrystalline andalusite-type AlFeGeO with 
to 
were performed. The magnetic Bragg peaks with the propagation vector of 
= (0, 0.150(1), 0) for the sample with and 
= (0, 0.141(1), 0) for the sample with 
were observed, which means that an incommensurate magnetic order was realized for each sample. The calculation of the magnetic structure factors by the Pawley method and the analysis of the irreducible representations revealed that both samples have a magnetic structure in which the magnetic moments rotate in the crystallographic 
-plane with sinusoidal modulation along the 
-axis. By the Luttinger Tisza method, we determined the sign of the nearest-neighbor exchange interaction consists that reproduce the magnetic structure obtained by the irreducible representation analysis.
Al and Nd
Pd
Ge
目時 直人; 柴田 薫; 松浦 直人*; 北澤 英明*; 鈴木 博之*; 山内 宏樹; 萩原 雅人; Frontzek, M. D.*; 松田 雅昌*
Journal of the Physical Society of Japan, 91(5), p.054710_1 - 054710_6, 2022/05
被引用回数：0 パーセンタイル：0.00(Physics, Multidisciplinary)NdPdAlにおけるNdの超微細相互作用分裂を高分解能の中性子非弾性散乱によって研究した。Nd核の核スピン(
=7/2)と、
の軌道が主成分の
基底状態を示す4
電子との間の超微細相互作用によって、磁気秩序相において生じた超微細相互作用分裂に起因する中性子非弾性散乱ピークを、
= 
3eVのエネルギーに観察した。低温では、Nd核スピンの低エネルギー状態の占拠確率が増加することによりNd核スピンが偏極し、反強磁性散乱ピーク強度に寄与するが、その際、中性子の非スピン反転過程の寄与が最も大きい。この現象の応用として反強磁性散乱ピーク強度の温度変化から、NdPdGeのNd磁気モーメント及び超微細相互作用分裂の大きさを見積もることに成功した。
SbO
F observed by high-resolution synchrotron and neutron diffraction下野 聖矢*; 石橋 広記*; 永吉 祐輔*; 池野 豪一*; 河口 彰吾*; 萩原 雅人; 鳥居 周輝*; 神山 崇*; 市橋 克哉*; 西原 禎文*; et al.
Journal of Physics and Chemistry of Solids, 163, p.110568_1 - 110568_7, 2022/04
被引用回数：1 パーセンタイル：13.39(Chemistry, Multidisciplinary)The structural phase transition from cubic (
) to a 
tetragonal (
) at 
180 K was found in non-centrosymmetric oxyfluoride CoSbOF by high-resolution neutron and synchrotron powder diffraction. To investigate this phase transition, specific heat, magnetization, and dielectric measurements were performed. Although the specific heat and dielectric constant showed anomalies at , a phase transition to ferroelectricity was not observed in the polarization hysteresis loop down to 30 K. The rotation of the CoOF octahedron was observed at from the structural analysis using synchrotron and neutron powder diffraction data. It was found that the magnetic phase transition from paramagnetic to G-type antiferromagnetic occurred at 67 K, at which a peak was observed in the specific heat measurements, via magnetic structure analysis using neutron powder diffraction data. The magnetic moments of Co
were aligned along the tetragonal 
-axis direction with a Co moment of 2.80(1) 
at 13 K.
and SrLaCuNbO; Spin-
quasi-square-lattice 
-
Heisenberg antiferromagnets渡邊 正理*; 栗田 伸之*; 田中 秀数*; 植野 航*; 松井 一樹*; 後藤 貴行*; 萩原 雅人
Physical Review B, 105(5), p.054414_1 - 054414_12, 2022/02
被引用回数：4 パーセンタイル：54.33(Materials Science, Multidisciplinary)We report the magnetic properties of the double perovskites SrLaCuSbO (SLCSO) and SrLaCuNbO (SLCNO). The temperature dependence of the magnetic susceptibilities of both com-pounds shows a broad maximum characteristic of an = 1/2 square lattice Heisenberg antiferromagnet. Magnetic ordering occurs at 
= 13.6 and 15.7 K for SLCSO and SLCNO, respectively. Neutron powder diffraction measurements reveal contrasting spin structures in both compounds. The spin structures of SLCSO and SLCNO below are N
el antiferromagnetic and collinear antiferromagnetic, respectively. This result demonstrates that the nearest-neighbor interaction is dominant in SLCSO, whereas the next-nearest-neighbor interaction is dominant in SLCNO. The magnitude of the ordered moment was evaluated at 3.5 K to be 
= 0.39(3) 
for SLCSO and 0.29(2) for SLCNO, which are significantly smaller than those calculated using linear spin wave theory. We infer that the small ordered moment is caused by the effect of exchange bond randomness arising from the site disorder of Sr and La ions.
林田 健志*; 上村 洋平*; 木村 健太*; 松岡 悟志*; 萩原 雅人; 廣瀬 左京*; 盛岡 仁*; 長谷川 達夫*; 木村 剛*
Physical Review Materials (Internet), 5(12), p.124409_1 - 124409_10, 2021/12
被引用回数：17 パーセンタイル：76.86(Materials Science, Multidisciplinary)The ferroaxial order, which is characterized by a rotational structural distortion in a crystal, has been recently proposed as one of ferroic orders. Though the domain formation is a characteristic feature in ferroic materials, there has been little study done concerning that for the ferroaxial order. Here, we investigate ferroaxial domains that are formed through a ferroaxial transition in two representative ferroaxial materials, NiTiO and RbFe(MoO). We spatially resolve their domain structures using an optical method based on electric-field- induced optical rotation, that is, electrogyration (EG). In NiTiO, multi-domains are constructed when crystals undergo a ferroaxial transition and the domain size depends on the cooling rate around the transition temperature. Furthermore, the ferroaxial domain structure obtained by the EG measurement is well matched with that by scanning X-ray diffraction (XRD). RbFe(MoO) also exhibits multi-domain states in which domain patterns are different each time a crystal undergoes a ferroaxial transition. In addition, the temperature dependence of the EG signal well obeys that of the order parameter of a first-order phase transition. These results ensure the effectiveness of the EG effect to elucidate the nature of ferroaxial order.
TaO木村 健太*; 八木 直輝*; 長谷川 舜介*; 萩原 雅人; 三宅 厚志*; 徳永 将史*; Cao, H.*; 益田 隆嗣*; 木村 剛*
Inorganic Chemistry, 60(20), p.15078 - 15084, 2021/10
被引用回数：1 パーセンタイル：9.44(Chemistry, Inorganic & Nuclear)In materials showing a linear magnetoelectric (ME) effect, unconventional functionalities can be anticipated such as electric control of magnetism and nonreciprocal optical responses. Thus, the search of new linear ME materials is of interest in materials science. Here, using a recently proposed design principle of linear ME materials, which is based on the combination of local structural asymmetry and collinear antiferromagnetism, we demonstrate that an anion-deficient fluorite derivative MnTaO is a new linear ME material. This is evidenced by the onset of magnetic-field-induced electric polarization in its collinear antiferromagnetic phase below = 24 K. Furthermore, we also find an antiferroelectric-like phase transition at = 55 K, which is attributable to an off-center displacement of magnetic Mn ions. The present study shows that MnTaO is a rare material that exhibits both ME and antiferroelectric-like transitions. Thus, MnTaO may provide an opportunity to investigate the physics associated with complicated interactions between magnetic (spin) and electric dipole degrees of freedom.
Wu, P.*; Fan, F.-R.*; 萩原 雅人*; 古府 麻衣子; Peng, K.*; 石川 喜久*; Lee, S.*; 本田 孝志*; 米村 雅雄*; 池田 一貴*; et al.
New Journal of Physics (Internet), 22(8), p.083083_1 - 083083_9, 2020/08
被引用回数：9 パーセンタイル：60.75(Physics, Multidisciplinary)熱電材料SnSeは、過去数年間で世界的な関心を呼び、その固有の強い格子非調和性は、その優れた熱電性能の重要な要素と見なされている。一方、SnSeにおける格子非調和性の理解は、特にフォノンダイナミクスがこの動作によってどのように影響を受けるかに関して、依然として不十分である。そのため、中性子全散乱,非弾性中性子散乱,ラマン分光法、および凍結フォノン計算により、Na
Sn
Se
S
の格子力学の包括的な研究を行った。格子非調和性は、対分布関数,非弾性中性子散乱、およびラマン測定によって確かめられた。熱膨張と多重フォノン散乱の影響を分離することにより、後者は高エネルギー光学フォノンモードで非常に重要であることがわかった。フォノンモードの強い温度依存性は、この系の非調和性を示している。さらに、我々のデータは、Sドーピングにより、高エネルギー光学フォノンの線幅が広がることを明らかにした。私たちの研究は、SnSeの熱電性能は、フォノンエンジニアリングを介して格子熱伝導率への高エネルギー光学フォノンモードの寄与を減らすことによってさらに強化できることを示唆する。
RhSi山内 宏樹; Sari, D. P.*; 渡邊 功雄*; 安井 幸夫*; Chang, L.-J.*; 近藤 啓悦; 伊藤 孝; 石角 元志*; 萩原 雅人*; Frontzek, M. D.*; et al.
Communications Materials (Internet), 1, p.43_1 - 43_6, 2020/07
中性子とミュオンの相補利用により、720Kまでの高温での短距離磁気秩序現象をMnRhSiで発見した。
ladder上田 宏*; 小野田 繁樹*; 山口 泰弘*; 木村 剛*; 吉澤 大智*; 森岡 俊晶*; 萩原 政幸*; 萩原 雅人*; 左右田 稔*; 益田 隆嗣*; et al.
Physical Review B, 101(14), p.140408_1 - 140408_6, 2020/04
被引用回数：4 パーセンタイル：25.35(Materials Science, Multidisciplinary)We report experimental and theoretical evidence that RbCuMoO
has a nonmagnetic tetramer ground state of a two-leg ladder comprising antiferromagnetically coupled frustrated spin- chains and exhibits a Haldane spin gap of emergent spin-1 pairs. Three spin excitations split from the spin-1 triplet by a Dzyaloshinskii-Moriya interaction are identified in inelastic neutron-scattering and electron spin resonance spectra. A tiny magnetic field generates ferroelectricity without closing the spin gap, indicating a unique class of ferroelectricity induced by a vector spin chirality order.
-electron state of the heavy fermion superconductor NpPdAl and the isostructural family目時 直人; Aczel, A. A.*; 青木 大*; Chi, S.*; Fernandez-Baca, J. A.*; Griveau, J.-C.*; 萩原 雅人*; Hong, T.*; 芳賀 芳範; 池内 和彦*; et al.
JPS Conference Proceedings (Internet), 30, p.011123_1 - 011123_6, 2020/03
希土類(4)やアクチノイド(5)は、電子数の増加とともに複雑さを増し、様々な相互作用が競合して多様な状態が出現する。多体電子系の結晶場分裂はバンド幅より狭いため、(1)高分解能の実験が必要で、(2)遍歴的なCeやU化合物は本質的に明瞭なスペクトルを示さない。また、(3)国際規制物質NpやPuなど超アクチノイド元素の取り扱いは厳しく規制されている。そこで比較的局在性の強い物質や希土類関連物質の、中性子散乱実験による磁気励起の研究が有益である。本稿では重い電子系化合物NpPdAlと関連物質の電子状態について述べる。
廣部 大地*; 佐藤 正寛*; 萩原 雅人*; 塩見 雄毅*; 益田 隆嗣*; 齊藤 英治
Physical Review Letters, 123(11), p.117202_1 - 117202_7, 2019/09
被引用回数：14 パーセンタイル：70.52(Physics, Multidisciplinary)Investigating exotic magnetic materials with spintronic techniques is effective at advancing magnetism as well as spintronics. In this work, we report unusual field-induced suppression of the spin Seebeck effect (SSE) in a quasi-one-dimensional frustrated spin- magnet LiCuVO, known to exhibit spin-nematic correlation in a wide range of external magnetic field 
. The suppression takes place above 
T in spite of the -linear isothermal magnetization curves in the same range. The result can be attributed to the growth of the spin-nematic correlation while increasing . The correlation stabilizes magnon pairs carrying spin 2, thereby suppressing the interfacial spin injection of SSE by preventing the spin-1 exchange between single magnons and conduction electrons at the interface. This interpretation is supported by integrating thermodynamic measurements and theoretical analysis on the SSE.
-electron states in PrPdAl目時 直人; 山内 宏樹; 鈴木 博之*; 北澤 英明*; 萩原 雅人*; 益田 隆嗣*; Aczel, A. A.*; Chi, S.*; Hong, T.*; 松田 雅昌*; et al.
Journal of the Physical Society of Japan, 87(9), p.094704_1 - 094704_8, 2018/09
被引用回数：6 パーセンタイル：46.04(Physics, Multidisciplinary)中性子非弾性散乱実験によりPrPdAlの電子状態を明らかにした。この物質のユニークな結晶構造に起因する2次元的な結晶場ポテンシャルにより、大きな
を伴う平べったい軌道が安定化し、イジング型の磁気異方性が生じることがわかった。この2次元的な結晶場ポテンシャルは同じ結晶構造を持つ希土類化合物RPdAlに共通に存在し、重い電子系超伝導体NpPdAlにおけるXY型磁気異方性への変化を系統的に説明することができる。それは、電子の局所的な性質がこの物質系の物性発現機構において非常に重要であり、NpPdAlにおける重い電子系超伝導にも関与している。
