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大塚 悠介*; 金澤 直也*; 平山 元昭*; 松井 彬*; 野本 拓也*; 有田 亮太郎*; 中島 多朗*; 花島 隆泰*; Ukleev, V.*; 青木 裕之; et al.
Science Advances (Internet), 7(47), p.eabj0498_1 - eabj0498_9, 2021/11
被引用回数：1 パーセンタイル：16.71(Multidisciplinary Sciences)FeSi is a nonmagnetic narrow-gap insulator, exhibiting peculiar charge and spin dynamics beyond a simple band structure picture. Those unusual features have been attracting renewed attention from topological aspects. Although the surface conduction was demonstrated according to size-dependent resistivity in bulk crystals, its topological characteristics and consequent electromagnetic responses remain elusive. Here, we demonstrate an inherent surface ferromagnetic-metal state of FeSi thin films and its strong spin-orbit coupling (SOC) properties through multiple characterizations of two-dimensional conductance, magnetization, and spintronic functionality. Terminated covalent bonding orbitals constitute the polar surface state with momentum-dependent spin textures due to Rashba-type spin splitting, as corroborated by unidirectional magnetoresistance measurements and first-principles calculations. As a consequence of the spin-momentum locking, nonequilibrium spin accumulation causes magnetization switching. These surface properties are closely related to the Zak phase of the bulk band topology. Our findings propose another route to explore noble metal-free materials for SOC-based spin manipulation.
丸山 龍治; 山崎 大; 青木 裕之; 阿久津 和宏*; 花島 隆泰*; 宮田 登*; 曽山 和彦; Bigault, T.*; Saerbeck, T.*; Courtois, P.*
Journal of Applied Physics, 130(8), p.083904_1 - 083904_10, 2021/08
被引用回数：2 パーセンタイル：34.91(Physics, Applied)Ferromagnetic (FM) interlayer exchange coupling of ion-beam sputtered Fe/Ge multilayers was investigated by off-specular polarized neutron scattering measurements. We observed a monotonously growing correlation of magnetic moments in the out-of-plane direction with decreasing Ge thickness. The results of the Fe/Ge multilayers were used to invoke FM interlayer exchange coupling in a neutron polarizing supermirror in order to extend its bandwidth. Typically, the bandwidth is limited due to a Curie temperature close to room temperature of the thinnest Fe layers with less than 3 nm. We propose a modified layer sequence of the neutron polarizing supermirror, where the minimum Fe thickness was set to 3.5 nm whereas the Ge thickness was reduced. A performance test of the neutron polarizing supermirror showed that the FM interlayer exchange coupling contributed to the presence of the magnetization comparable to the bulk and resulted in a marked extension in the bandwidth.
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.
丸山 龍治; 山崎 大; 阿久津 和宏*; 花島 隆泰*; 宮田 登*; 青木 裕之; 曽山 和彦
JPS Conference Proceedings (Internet), 33, p.011092_1 - 011092_6, 2021/03
中性子偏極スーパーミラーは、熱及び冷中性子ビームを偏極するための光学素子であり、実機への応用には高偏極率であるとともに必要な外部磁場を小さく抑えること、即ち偏極スーパーミラーを構成する磁気多層膜が磁気的にソフトであることが重要である。本発表では、J-PARC MLFの共用ビームラインBL17等を用いて得られた偏極スーパーミラーの高偏極率化、及び磁気多層膜の軟磁性化を目指しこれを構成する多層膜特有の磁気特性の解明に関する成果について議論する。
阿久津 和宏*; 吉良 弘*; 宮田 登*; 花島 隆泰*; 宮崎 司*; 笠井 聡*; 山崎 大; 曽山 和彦; 青木 裕之
Polymers (Internet), 12(10), p.2180_1 - 2180_10, 2020/10
被引用回数：2 パーセンタイル：11.82(Polymer Science)A large background scattering originating from the sample matrix is a major obstacle for fine-structure analysis of a nanometric layer buried in a bulk material. As polarization analysis can decrease undesired scattering in a neutron reflectivity (NR) profile, we performed NR experiments with polarization analysis on a polypropylene (PP)/perhydropolysilazane-derived SiO
(PDS)/Si substrate sample, having a deep-buried layer of SiO to elucidate the fine structure of the nano-PDS layer. This method offers unique possibilities for increasing the amplitude of the Kiessig fringes in the higher scattering vector (Qz) region of the NR profiles in the sample by decreasing the undesired background scattering. Fitting and Fourier transform analysis results of the NR data indicated that the synthesized PDS layer remained between the PP plate and Si substrate with a thickness of approximately 109 
;. Furthermore, the scattering length density of the PDS layer, obtained from the background subtracted data appeared to be more accurate than that obtained from the raw data. Although the density of the PDS layer was lower than that of natural SiO, the PDS thin layer had adequate mechanical strength to maintain a uniform PDS layer in the depth-direction under the deep-buried condition.
池田 修悟*; 金子 耕士; 田中 佑季*; 川崎 卓郎; 花島 隆泰*; 宗像 孝司*; 中尾 朗子*; 鬼柳 亮嗣; 大原 高志; 望月 健生*; et al.
Journal of the Physical Society of Japan, 89(1), p.014707_1 - 014707_7, 2020/01
被引用回数：0 パーセンタイル：0(Physics, Multidisciplinary)Magnetism in EuNiIn has been studied by specific heat, magnetic susceptibility, magnetization, 
Eu M
ssbauer spectroscopy, and neutron diffraction experiments. The specific heat shows two magnetic transitions at 
and 
at zero magnetic field. An antiferromagnetic ground state of EuNiIn has a uniaxial magnetic anisotropy along the b-axis, revealed by the magnetic susceptibility and the Mssbauer spectroscopy. Single crystal neutron diffraction experiments clarify that this antiferromagnetic structure in the ground state is characterized by the commensurate propagation vector 
= (1/2, 1/2, 1/2) which reveals no distinct anomaly at . The magnetization curve along the b-axis at 2 K shows four successive magnetic field-induced transitions up to 50 kOe and, reaches 7 
/f.u. above 190 kOe, The magnetic phase diagram in EuNiIn has unique characteristics with five magnetic states in low magnetic field.
川北 至信; 菊地 龍弥*; 稲村 泰弘; 田原 周太*; 丸山 健二*; 花島 隆泰*; 中村 充孝; 鬼柳 亮嗣; 山内 康弘*; 千葉 薫*; et al.
Physica B; Condensed Matter, 551, p.291 - 296, 2018/12
被引用回数：9 パーセンタイル：47.49(Physics, Condensed Matter)単元素液体金属の中には、その静的構造が剛体球充填モデルでは全く表せない、複雑な構造を有する物質がある。液体ビスマスは、構造因子のメインピークの高波数側に非対称な肩構造を有する。二体分布関数の第一ピークと第二ピークの距離の比が1:2で、一次元的に配列しているような奇妙な値を示すとともに、第一ピークの長距離側に明確な肩構造を有する。二種類の直径の異なる剛体球からなるモデルでは、構造因子の肩構造が生じることから、こうした単元素液体金属の複雑性の起源として、短時間だけ生じる共有結合や、金属イオンを遮蔽する電子が有効二体間ポテンシャルに作り出す振動(フリーデル振動)など、まったく物理的描像が異なる仮説がいくつかなされている。そこで我々は液体ビスマスの中性子準弾性散乱を、J-PARCのMLFに設置された冷中性子ディスクチョッパー分光器を用いて測定し、液体ダイナミクスを動的相関関数から調べた。その結果、二体分布関数の第一ピークの肩構造の緩和時間が、第一ピークや第二ピークなどその他の主要構造に比べて著しく長いことが分かった。
(Si
[]
)O
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
被引用回数：21 パーセンタイル：68.59(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
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(Si[]])O instead of the interstitial oxygens, by single-crystal neutron and X-ray diffraction analyses, density measurements and 
electronic calculations.
S
films; Case of pre-reaction坂口 佳史*; 花島 隆泰*; 青木 裕之; 朝岡 秀人; Simon, A.-A. A.*; Mitkova, M.*
Physica Status Solidi (A), 215(12), p.1800049_1 - 1800049_12, 2018/06
被引用回数：5 パーセンタイル：29.93(Materials Science, Multidisciplinary)Silver photodiffusion into amorphous chalcogenide has attracted much attention because of its potential applications for example in memory devices. For its development, it is important to know how Ag ions diffuse in chalcogenide layers upon light exposure. In this paper, the photo-induced effect on pre-reacted films before light exposure, originating from Ag/GeS/Si substrate and GeS/Ag/Si substrate is investigated, using neutron reflectivity, X-ray reflectivity, and X-ray diffraction. Two types of pre-reacted films according to the original stacking order are obtained. In both cases, a pure Ag layer almost disappeared, and there is a small amount of monoclinic AgS. The reaction time for the photodiffusion is shorter, in both cases, than that in Ag/GeS with a pure Ag layer, indicating a different reaction process. After prolonged light exposure, a uniform amorphous reaction layer is produced in the films originating from the Ag/GeS/Si substrate, while both an amorphous reaction product and the AgS fragments exist in the films originating from GeS/Ag/Si substrate. The mechanism of the specific photo-reaction is discussed in terms of the role of the AgS fragments.
丸山 龍治; 山崎 大; 阿久津 和宏*; 花島 隆泰*; 宮田 登*; 青木 裕之; 武田 全康; 曽山 和彦
Nuclear Instruments and Methods in Physics Research A, 888, p.70 - 78, 2018/04
被引用回数：3 パーセンタイル：35.39(Instruments & Instrumentation)イオンビームスパッタ法で成膜されたFe/Si及びFe/Ge多層膜に対して、X線及び偏極中性子反射率、走査型透過電子顕微鏡と組み合わされたエネルギー分散型X線分光分析等のプローブによって層構造や局所元素分析を行った。その結果、Fe/Ge多層膜のGe層に含まれたスパッタリングガスであるArが含まれることにより、Ge層の散乱長密度が減少し、(-)スピンの中性子に対するFeとGeの散乱長密度のコントラストがほぼ消失し偏極中性子反射において高偏極率となることがわかった。Ge層に含まれるArは、成膜時においてAeがGeターゲットで後方散乱することに起因することが知られており、偏極スーパーミラーの高偏極率化に必要な(-)スピン中性子に対する散乱長密度コントラストを微調整する新たな手法となる可能性を示すものである。この結果を基に、Niの5倍の全反射臨界角をもつFe/Ge偏極スーパーミラーを成膜し偏極反射率測定を行った結果、(+)スピン中性子の反射率が0.70以上、偏極率はビームラインの偏極性能が正しく補正されている領域においては0.985以上という高い偏極率を達成した。
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
被引用回数：21 パーセンタイル：63.15(Multidisciplinary Sciences)Orthosilicic acid (Si(OH)
) 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.
studied by single-crystal time-of-flight neutron diffraction川崎 卓郎; 金子 耕士; 仲村 愛*; 阿曽 尚文*; 辺土 正人*; 仲間 隆男*; 大原 高志; 鬼柳 亮嗣; 及川 健一; 田村 格良; et al.
Journal of the Physical Society of Japan, 85(11), p.114711_1 - 114711_5, 2016/11
被引用回数：8 パーセンタイル：55.05(Physics, Multidisciplinary)The magnetic structure of the intermetallic compound EuGa was investigated using single-crystal neutron diffraction with TOF Laue technique on the new diffractometer SENJU at MLF of J-PARC. Despite of the high neutron absorption of Eu, a vast number of diffraction spots were observed without isotope enrichment. The magnetic reflections appeared at 
2
below 16 K, indicating that the ordering vector is = (0, 0, 0). The continuous evolution of the magnetic reflection intensity below T
follows a squared Brillouin function for 
= 7/2. By adopting a wavelength-dependent absorption collection, the magnetic structure of EuGa revealed that a nearly full magnetic moment of 6.4 
B of Eu lies within the basal plane of the lattice.
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
被引用回数：44 パーセンタイル：95.7(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 crystal were performed to evaluate its performance.
NbO
Khanh, N. D.*; 阿部 伸行*; 佐賀山 基*; 中尾 朗子*; 花島 隆泰*; 鬼柳 亮嗣; 徳永 祐介*; 有馬 孝尚*
Physical Review B, 93(7), p.075117_1 - 075117_6, 2016/02
被引用回数：90 パーセンタイル：95.22(Materials Science, Multidisciplinary)The magnetic structure and magnetoelectric effect have been investigated for single crystals of the antiferromagnet CoNbO. Single-crystal neutron diffraction and magnetic susceptibility measurement have revealed that the magnetic structure is different from a collinear arrangement with spin parallel to the trigonal axis as proposed previously. Co
magnetic moments are found to be almost lying in the basal plane, which lowers the magnetic symmetry to 
with the propagation vector 
= 0. Associated with the magnetic phase transition, a sharp anomaly in the dielectric constant and displacement current indicate the appearance of the magnetoelectric below Neel temperature TN with a large coupling constant up to 30 ps/m. The existence of off-diagonal components in a magnetoelectric tensor indicate the formation of ferrotoroidic order in CoNbO. Such a magnetoelectric effect can be ascribed to the reduction of symmetry caused by simple antiferromagnetic order in a honeycomb network.
-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
被引用回数：6 パーセンタイル：23.65(Chemistry, Multidisciplinary)A newly synthesized one-dimensional (1D) hydrogen-bonded (H-bonded) rhodium(II)--semiquinone complex, [Cp
Rh(-
-HSQ-Me)]PF
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 ion. The relative permittivity 
' along the H-bonded chains reaches relatively high values (ca., 130) in the RT phase.
及川 健一; 川崎 卓郎; 大原 高志; 鬼柳 亮嗣; 金子 耕士; 田村 格良; 中村 龍也; 原田 正英; 中尾 朗子*; 花島 隆泰*; et al.
JPS Conference Proceedings (Internet), 1, p.014013_1 - 014013_5, 2014/03
新しいTOF型単結晶中性子回折装置がJ-PARC/MLFのBL18に設置された。本装置「SENJU」は、低温高磁場のような多重極限環境下において1.0mm
未満の小さな単結晶を使用して精密な結晶構造や磁気構造解析を実現するために設計された。2012年3月5日に、本装置へ初中性子が導かれ、その後SENJUのハードウェア及びソフトウェアが設計通り機能していることが確認された。また、幾つかの有機及び無機の標準的な単結晶を用いて回折実験が行われた。これらの測定では、高いQ領域(d
0.5 
のブラッグ反射が明確に測定され、精度よく解析された。発表では、SENJUの装置設計及びその性能評価を詳細に報告する。
川崎 卓郎; 金子 耕士; 阿曽 尚文*; 仲村 愛*; 辺土 正人*; 仲間 隆男*; 大貫 惇睦*; 大原 高志; 鬼柳 亮嗣; 及川 健一; et al.
JPS Conference Proceedings (Internet), 1, p.014009_1 - 014009_4, 2014/03
Single crystal neutron diffraction measurement of EuGa has been carried out using time-of-flight single crystal neutron diffractometer SENJU at BL18 in MLF/J-PARC. In spite of extremely high neutron absorption of natural Eu, significant numbers of Bragg reflection were observed. Lattice parameters and Bravais lattice at above 
(=15 K) obtained from the positions and systematic extinction of the reflections were well agreed with the result of single crystal X-ray diffraction. Further, magnetic reflections were clearly observed at below at the positions of forbidden reflections of body-centered lattice of EuGa. An antiferromagnetic structure with the propagation vector = 0 was clarified.
及川 健一; 大原 高志*; 鬼柳 亮嗣; 川崎 卓郎; 田村 格良; 金子 耕士; 木村 宏之*; 野田 幸男*; 高橋 美和子*; 清谷 多美子*; et al.
no journal, ,
J-PARCのBL18では、共用促進法に基づき、新しい単結晶構造解析装置SENJUが急ピッチで建設されている。SENJUは、1MWにおいて0.5mm角の単結晶を用いた実験を可能とし、中性子が得意とする複合特殊環境下での精密構造解析を目指す装置である。単結晶試料のサイズ及びモザイシティ、検出器の実空間分解能を含めた装置デザインの中でビームラインの仕様を決定した。具体的な設計入力としては、(1)標準的な入射ビーム発散角は
とし
まで利用する、(2)高強度モードでは
を目標とし
まで利用する、(3)モデレータからの即発
線は試料位置で10kcps/
以下とする、(4)試料位置での一様なビームサイズは3mm角程度とする、(5)真空散乱槽内でのビームハローは40mm角以下とする、(6)フレームオーバーラップ成分の混入を避ける、などである。当日は、これら検討プロセス及びその結果の詳細仕様について述べる。
鬼柳 亮嗣; 及川 健一; 田村 格良; 大原 高志; 川崎 卓郎; 金子 耕士; 中尾 朗子*; 花島 隆泰*; 宗像 孝司*; 木村 宏之*; et al.
no journal, ,
A new time-of-flight single crystal diffractometer, SENJU, is being constructed in Materials and Life Science Experimental Facility (MLF) at Japan Proton Accelerator Research Complex (J-PARC). This instrument aims to pursue precise crystal and magnetic structure analyses of the small samples with the lattice constants up to 50. Available sample environments will include low temperature, high magnetic field and high pressure. A superconducting magnet has a wide opening angle for diffracted neutrons and a large bore around sample area. A dilution refrigerator (
50 mK) can be mounted onto the magnet. Other ancillary equipment can be also utilized in combination with another. Softwares were also developed based on the software "STARGazer" that has been developed for iBIX at J-PARC. New features such as controlling goniometers and ancillary equipment, live-monitoring of measurements and the reconstruction of a intensity distribution in 3D reciprocal space were introduced.
及川 健一; 大原 高志*; 鬼柳 亮嗣; 川崎 卓郎; 田村 格良; 金子 耕士; 中村 龍也; 坂佐井 馨; 中尾 朗子*; 花島 隆泰*; et al.
no journal, ,
千手観音から名前を頂いたSENJUは、J-PARCのMLFに提案されたTOF型の単結晶ラウエ回折装置である。SENJUは、結晶構造及び磁気構造の精密解析を、多重極限下において行うことに特化した装置であり、1 
以下の小さな試料を測定に用いる。TOF型ラウエ法と広角二次元検出器の組合せにより、効率的な測定を実現するとともに、データの完全性を改善できる。波長変換方式のシンチレーション検出器はiBIXのために開発されたものであるが、これをSENJUの要求仕様に合わせ改良した。SENJUの建設スケジュールは地震により遅れたが、オンビームコミッショニングは2012年早々に開始される予定である。
