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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, 48(1), p.333 - 338, 2019/01

 パーセンタイル:100(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.


Unique helical magnetic order and field-induced phase in trillium lattice antiferromagnet EuPtSi

金子 耕士; Frontzek, M. D.*; 松田 雅昌*; 中尾 朗子*; 宗像 孝司*; 大原 高志; 垣花 将司*; 芳賀 芳範; 辺土 正人*; 仲間 隆男*; et al.

Journal of the Physical Society of Japan, 88, p.013702_1 - 013702_5, 2019/01

 被引用回数:1 パーセンタイル:14.05(Physics, Multidisciplinary)

Magnetic transitions in chiral antiferromagnet EuPtSi were investigated by means of single crystal neutron diffraction. In the ground state, magnetic peaks emerge at positions represented by $$q_{1}$$=$$(0.2, 0.3, 0)$$. Upon heating, an additional magnetic peak splitting around 2.5 K was uncovered, indicating a presence of a first-order transition with $$q^*_{1}$$=$$(0.2, 0.3, {delta})$$. An half-polarized neutron scattering for polarization parallel to Q reveled that polarization antiparallel to Q has stronger intensity in both magnetic phases. This feature clarifies single chiral character of helical structure with moments normal to the ordering vector in both ordered states. Under vertical magnetic field along [1,1,1] in the $$A$$ phase, magnetic peaks form hexagonal patterns in the equatorial scattering plane around nuclear. An ordering vector $$q_{A}$$ of the $$A$$-phase has the similar size in the periodicity to $$q_{1}$$, and could be a hallmark of a formation of skyrmion lattice in EuPtSi.


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

 パーセンタイル:100(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 N$'e$el temperature $$T_{rm N}$$ $$approx$$ 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.


Mn$$_{2}$$VAl Heusler alloy thin films; Appearance of antiferromagnetism and exchange bias in a layered structure with Fe

土屋 朋生*; 小林 亮太*; 窪田 崇秀*; 斉藤 耕太郎*; 小野 寛太*; 大原 高志; 中尾 朗子*; 高梨 弘毅*

Journal of Physics D; Applied Physics, 51(6), p.065001_1 - 065001_7, 2018/02

 被引用回数:1 パーセンタイル:100(Physics, Applied)

Mn$$_{2}$$VAl Heusler alloy films were epitaxially grown on MgO(100) single-crystal substrates by ultra-high-vacuum magnetron sputtering. A2- and L21-type Mn$$_{2}$$VAl order was controlled by the deposition temperature. A2-type Mn$$_{2}$$VAl films showed no spontaneous magnetization, while L21-type Mn$$_{2}$$VAl films showed ferrimagnetic behaviour with a maximum saturation magnetization of 220 emu/cm$$^{3}$$ at room temperature (RT). An antiferromagnetic reflection was observed with neutron diffraction at RT for an A2-type Mn$$_{2}$$VAl film deposited at 400$$^{circ}$$C. A bilayer sample of the antiferromagnetic A2-type Mn$$_{2}$$VAl and Fe showed an exchange bias of 120 Oe at 10 K.


Neutron scattering study of yttrium iron garnet

社本 真一; 伊藤 孝; 大西 弘明; 山内 宏樹; 稲村 泰弘; 松浦 直人*; 赤津 光洋*; 樹神 克明; 中尾 朗子*; 茂吉 武人*; et al.

Physical Review B, 97(5), p.054429_1 - 054429_9, 2018/02

 被引用回数:1 パーセンタイル:100(Materials Science, Multidisciplinary)



Materials and Life Science Experimental Facility (MLF) at the Japan Proton Accelerator Research Complex, 2; Neutron scattering instruments

中島 健次; 川北 至信; 伊藤 晋一*; 阿部 淳*; 相澤 一也; 青木 裕之; 遠藤 仁*; 藤田 全基*; 舟越 賢一*; Gong, W.*; et al.

Quantum Beam Science (Internet), 1(3), p.9_1 - 9_59, 2017/12



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

 被引用回数:2 パーセンタイル:70.98(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.


Magnetic structure of divalent europium compound EuGa$$_{4}$$ 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

 パーセンタイル:100(Physics, Multidisciplinary)

The magnetic structure of the intermetallic compound EuGa$$_{4}$$ 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 $$h + k + l$$ $$neq$$ 2$$n$$ below 16 K, indicating that the ordering vector is $$q$$ = (0, 0, 0). The continuous evolution of the magnetic reflection intensity below T$$_{N}$$ follows a squared Brillouin function for $$S$$ = 7/2. By adopting a wavelength-dependent absorption collection, the magnetic structure of EuGa$$_{4}$$ revealed that a nearly full magnetic moment of 6.4 $$mu$$B of Eu lies within the basal plane of the lattice.


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

 被引用回数:13 パーセンタイル:9.6(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.


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

 被引用回数:13 パーセンタイル:11.41(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.


Magnetoelectric coupling in the honeycomb antiferromagnet Co$$_{4}$$Nb$$_{2}$$O$$_{9}$$

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, p.075117_1 - 075117_6, 2016/02

 被引用回数:33 パーセンタイル:5.52(Materials Science, Multidisciplinary)

The magnetic structure and magnetoelectric effect have been investigated for single crystals of the antiferromagnet Co$$_{4}$$Nb$$_{2}$$O$$_{9}$$. 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$$^{2+}$$ magnetic moments are found to be almost lying in the basal plane, which lowers the magnetic symmetry to $$C2/c'$$ with the propagation vector $$k$$ = 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 Co$$_{4}$$Nb$$_{2}$$O$$_{9}$$. Such a magnetoelectric effect can be ascribed to the reduction of symmetry caused by simple antiferromagnetic order in a honeycomb network.


Instrument design and performance evaluation of a new single crystal neutron diffractometer SENJU at J-PARC

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$$^3$$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 $AA)$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。


Single crystal neutron diffraction study of high neutron absorbing compound EuGa$$_{4}$$

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$$_{4}$$ 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 $$T_mathrm{N}$$ (=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 $$T_mathrm{N}$$ at the positions of forbidden reflections of body-centered lattice of EuGa$$_{4}$$. An antiferromagnetic structure with the propagation vector $$q$$ = 0 was clarified.


Spin state of Co$$^{3+} $$ in LaCo$$_{1-x}$$ Rh$$_{x}$$O$$_{3}$$ investigated by structural phenomena

浅井 晋一郎*; 岡崎 竜二*; 寺崎 一郎*; 安井 幸夫*; 小林 航*; 中尾 朗子*; 小林 賢介*; 熊井 玲児*; 中尾 裕則*; 村上 洋一*; et al.

Journal of the Physical Society of Japan, 82(11), p.114606_1 - 114606_6, 2013/11

 被引用回数:6 パーセンタイル:46.59(Physics, Multidisciplinary)

LaCo$$_{1-x}$$ Rh$$_{x}$$O$$_{3}$$について中性子および放射光X線回折実験を行い、Co$$^{3+}$$イオンのスピン状態と結晶構造との関連を調べた。10KにおけるLaCo$$_{0.8}$$Rh$$_{0.2}$$O$$_{3}$$では、Co(Rh)O$$_{6}$$八面体のCo(Rh)-O間距離は理論値と一致し、格子体積は温度低下によって減少した。また、この格子体積の減少に伴って高スピン状態の比率は減少した。これらの結果から、Co$$^{3+}$$イオンのスピン状態は高スピン状態と低スピン状態が混在したものであり、高スピン状態は、Rh$$^{3+}$$イオンの置換によって生じたピン止め効果に加え熱励起によって発現することがわかった。


Emergent phenomena in perovskite-type manganites

田口 康二郎*; 酒井 英明*; 奥山 大輔*; 石渡 晋太郎*; 藤岡 淳*; 福田 竜生; 橋爪 大輔*; 賀川 史敬*; 高橋 陽太郎*; 島野 亮*; et al.

Physica B; Condensed Matter, 407(11), p.1685 - 1688, 2012/06

 被引用回数:3 パーセンタイル:79.94(Physics, Condensed Matter)

Perovskite-type manganites exhibit various interesting phenomena arising from complex interplay among spin, charge, orbital, and lattice degrees of freedom. As the respective examples, perovskite-type YMnO$$_3$$ and Sr$$_{1-x}$$Ba$$_x$$MnO$$_3$$ are discussed. In the YMnO$$_3$$, the ferroelectric lattice distortion associated with the $$E$$-type spin order is observed for the first time. Displacement-type ferroelectricity with off-center magnetic ions is discovered for Sr$$_{0.5}$$Ba$$_{0.5}$$MnO$$_3$$, which shows both large polarization value and strong coupling between ferroelectricity and magnetism.



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, , 



Construction of new time-of-flight single crystal diffractometer SENJU at J-PARC

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${AA}$. 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 ($$sim$$ 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.


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

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 $$mm^3$$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。


Detector system of single crystal diffractometer SENJU

川崎 卓郎; 中村 龍也; 坂佐井 馨; 藤 健太郎; 細谷 孝明*; 曽山 和彦; 片桐 政樹*; 及川 健一; 金子 耕士; 田村 格良; et al.

no journal, , 

A novel time-of-flight single crystal neutron diffractometer, SENJU, is being constructed in MLF at J-PARC. The diffractometer will have 37 two-dimensional WLSF-type scintillator detectors to cover wide area of reciprocal lattice space by a single measurement. SENJU will receive first neutron in early 2012 in which 30 detectors will be installed around the sample chamber in a cylindrical arrangement and one detector will be installed just under the chamber. The maximum total covered solid angle around the sample will be 4.8 sr, which enables the efficient measurements and improves the completeness of the data. The detector for SENJU was developed based on the detector for iBIX to meet the requirement of SENJU, i.e. spatial resolution, chassis size, sensitive area and magnetic field tolerance. The 31 detectors have been already manufactured and their performances were tested by checking sources. Overview of the system and the performances of the detectors will be presented.



川崎 卓郎; 及川 健一; 大原 高志*; 鬼柳 亮嗣; 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, , 


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