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論文

Sorption behavior of selenide on montmorillonite

杉浦 佑樹; 戸村 努*; 石寺 孝充; 土井 玲祐; Francisco, P. C. M.; 塩飽 秀啓; 小林 徹; 松村 大樹; 高橋 嘉夫*; 舘 幸男

Journal of Radioanalytical and Nuclear Chemistry, 324(2), p.615 - 622, 2020/05

 被引用回数:0 パーセンタイル:100(Chemistry, Analytical)

Batch sorption experiments were performed to investigate the sorption mechanism of Se on montmorillonite under reducing conditions in deep geological environments. Based on Eh-pH diagrams and ultraviolet-visible spectra, Se was dissolved as selenide (Se(-II)) anions under the experimental conditions. The distribution coefficients ($$K_{rm d}$$; m$$^{3}$$ kg$$^{-1}$$) of Se(-II) indicated ionic strength independence and slight pH dependence. The $$K_{rm d}$$ values of Se(-II) were higher than those of Se(IV), which also exists as an anionic species. X-ray absorption near edge spectroscopy showed that the oxidation state of Se-sorbed on montmorillonite was zero even though selenide remained in the solution. These results suggest that Se(-II) was oxidized and precipitated on the montmorillonite surface. Therefore, it is implied that a redox reaction on the montmorillonite surface contributed to high $$K_{rm d}$$ values for Se(-II).

論文

Nature of structural instabilities in superconducting Sr$$_3$$Ir$$_4$$Sn$$_{13}$$

金子 耕士; Cheung, Y. W.*; Hu, Y.*; 今井 正樹*; 谷奥 泰明*; 金川 響*; 村川 譲一*; 森山 広大*; Zhang, W.*; Lai, K. T.*; et al.

JPS Conference Proceedings (Internet), 30, p.011032_1 - 011032_6, 2020/03

A quantum critical point appears as a second-order phase transition which takes place at zero temperature. In contrast to heavy-fermion systems in which magnetism often plays a vital role, recent studies revealed that structural instabilities can drive a system to a quantum critical point as well. In quasi-skutterudite (Ca,Sr)$$_3T_4$$Sn$$_{13}$$ ($$T$$=Rh, Ir), Sr$$_3$$Ir$$_4$$Sn$$_{13}$$ exhibits superconductivity around $$T_{rm sc}$$$${sim}$$5 K and a structural transition at $$T^*{simeq}$$147 K. Applying physical or chemical pressure on Sr$$_3$$Ir$$_4$$Sn$$_{13}$$ suppresses $$T^*$$ rapidly, and a quasi-linear $$T$$ dependence of electrical resistivity, signature of non-Fermi liquid behavior, was observed where $$T^*$$ extrapolates to 0~K. The isomorphs (Ca$$_x$$Sr$$_{1-x}$$)$$_3$$Rh$$_4$$Sn$$_{13}$$ exhibits similar behavior, where the criticality can be reached by $$x{sim}$$0.9 without external pressure. Neutron scattering experiments in Sr$$_3$$Ir$$_4$$Sn$$_{13}$$ evidences the second order nature of the structural transition at $$T^*$$ by the observation of a continuous evolution of superlattice peak below $$T^*$$ and a gradual increase of critical scattering upon approaching to $$T^*$$ by cooling. Increase of $$x$$ in (Ca$$_x$$Sr$$_{1-x}$$)$$_3$$Rh$$_4$$Sn$$_{13}$$ toward the quantum critical point leads to the systematic variation of the critical exponents of the order parameter. In addition, this substitution induces the phonon softening around the M point towards zero energy revealed by inelastic X-ray scattering experiment. We will present systematic variations in both elastic and inelastic channels upon approaching to the quantum critical point.

論文

Manipulation of saturation magnetization and perpendicular magnetic anisotropy in epitaxial Co$$_{x}$$Mn$$_{4-x}$$N films with ferrimagnetic compensation

伊藤 啓太*; 安富 陽子*; Zhu, S.*; Nurmamat, M.*; 田原 昌樹*; 都甲 薫*; 秋山 了太*; 竹田 幸治; 斎藤 祐児; 小口 多美夫*; et al.

Physical Review B, 101(10), p.104401_1 - 104401_8, 2020/03

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

Spintronics devices utilizing a magnetic domain wall motion have attracted increasing attention, and ferrimagentic materials with almost compensated magnetic moments are highly required to realize the fast magnetic domain wall motion. Here, we report a key function for this purpose in anti-perovskite Co$$_{x}$$Mn$$_{4-x}$$N films. Perpendicular magnetization emerges for $$0.8 leq x$$, and the saturation magnetization reaches a minimum value at $$x = 0.8$$.

論文

Zeolitic vanadomolybdates as high-performance cathode-active materials for sodium-ion batteries

Zhang, Z,*; Wang, H.*; 吉川 浩史*; 松村 大樹; 畑尾 秀哉*; 石川 理史*; 上田 渉*

ACS Applied Materials & Interfaces, 12(5), p.6056 - 6063, 2020/02

 被引用回数:0 パーセンタイル:100(Nanoscience & Nanotechnology)

Developing new cathode-active materials for rechargeable batteries is important to fulfill the growing demands of energy transformation, storage, and utilization. Zeolitic transition-metal oxides based on vanadomolybdate, constructed by pentagon metal-oxygen clusters as building blocks and metal ions as linkers in a trigonal symmetry, are good candidates for cathodes of Na rechargeable batteries. The material is activated via amorphization of the crystal structure in the ab plane during discharging process, keeping the molecular structure of the building blocks stable, which causes high specific capacity and good cycle performance.

論文

Anomalous small-angle X-ray scattering (ASAXS) study of irradiation-induced nanostructure change in Fe-ion beam irradiated oxide dispersion-strengthened (ODS) steel

熊田 高之; 大場 洋次郎; 元川 竜平; 諸岡 聡; 冨永 亜希; 谷田 肇; 菖蒲 敬久; 金野 杏彩; 大和田 謙二*; 大野 直子*; et al.

Journal of Nuclear Materials, 528, p.151890_1 - 151890_7, 2020/01

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

ステンレス鋼の放射線照射によるナノ構造変化観測用異常分散X線小角散乱(ASAXS)装置を開発した。イオンビーム照射前後のMA956試料の散乱パターンを比較したところ、Cr析出物の形状は全く変化していないことが判明した。

論文

Lattice dynamics in FeSe via inelastic X-ray scattering and first-principles calculations

村井 直樹; 福田 竜生; 中島 正道*; 河村 光晶*; 石川 大介*; 田島 節子*; Baron, A. Q. R.*

Physical Review B, 101(3), p.035126_1 - 035126_6, 2020/01

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

非弾性X線散乱を用いたFeSe超伝導体のフォノン研究について報告する。実験的に決定したフォノン分散と非磁性相の密度汎関数理論(DFT)とを比較を行うと、両所の間には顕著な不一致が見られた。FeSeは磁気秩序を示さないにもかかわらず、スピン偏極DFTを用いることによって初めて実験結果は再現される。この解析は、強いスピン揺らぎを内在した常時性状態における近似を与える。

論文

最先端放射光ナノ計測・解析共用拠点(日本原子力研究開発機構)

米田 安宏; 吉越 章隆; 竹田 幸治; 塩飽 秀啓; 松村 大樹; 菖蒲 敬久; 田村 和久

まてりあ, 58(12), p.763 - 769, 2019/12

文部科学省ナノプラットフォーム委託事業において、微細構造解析プラットフォームに属する各実施機関の提供している装置紹介である。

論文

X-ray absorption spectroscopy and magnetocaloric study of Pr$$_{1-x}$$Sr$$_{x}$$CoO$$_{3}$$ (0$$leq x leq$$0.5)

松村 大樹; 辻 卓也; 吉井 賢資

Materials Chemistry and Physics, 238, p.121885_1 - 121885_5, 2019/12

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

ペロブスカイトPr$$_{1-x}$$Sr$$_{x}$$CoO$$_{3}$$(0$$leq x leq$$0.5)についてX線吸収分光測定を行うとともに、x=0.5で観測される110Kの磁気異常の起源を探るため磁気熱量効果測定を行った。Co${it K}$吸収端のX線吸収測定からは、xが増えるとともにCoの原子価が増加し、Co-O結合距離が縮まることが分かった。また、CoO$$_{6}$$多面体の歪みも増大することが分かった。Co-O結合距離の縮み方は、xが大きいほど大きいことも分かった。測定温度範囲である17-300Kでは、Co${it K}$吸収端の吸収スペクトルには異常は見られなかった。磁気熱量効果の結果と合わせ、110Kの異常は磁気構造の変化であることが分かった。

論文

Intrinsic 2D ferromagnetism in V$$_{5}$$Se$$_{8}$$ epitaxial thin films

中野 匡規*; Wang, Y.*; 吉田 訓*; 松岡 秀樹*; 真島 裕貴*; 池田 啓祐*; 平田 靖透*; 竹田 幸治; 和達 大樹*; 小濱 芳允*; et al.

Nano Letters, 19(12), p.8806 - 8810, 2019/12

 被引用回数:2 パーセンタイル:60.62(Chemistry, Multidisciplinary)

The discoveries of intrinsic ferromagnetism in atomically thin van der Waals crystals have opened a new research field enabling fundamental studies on magnetism at two-dimensional (2D) limit as well as development of magnetic van der Waals heterostructures. Here we demonstrate that V$$_{5}$$Se$$_{8}$$ epitaxial thin films grown by molecular-beam epitaxy exhibit emergent 2D ferromagnetism with intrinsic spin polarization of the V 3d electrons although the bulk counterpart is originally antiferromagnetic. Moreover, thickness-dependence measurements reveal that this newly developed 2D ferromagnet could be classified as an itinerant 2D Heisenberg ferromagnet with weak magnetic anisotropy.

論文

Short- and middle-ranges order structures of KNbO$$_3$$ nanocrystals

米田 安宏; 國定 諒一*; 近田 司*; 上野 慎太郎*; 藤井 一郎*; 永田 肇*; 尾原 幸治*; 和田 智志*

Japanese Journal of Applied Physics, 58(SL), p.SLLA03_1 - SLLA03_7, 2019/11

 被引用回数:0 パーセンタイル:100(Physics, Applied)

We studied KNbO$$_3$$ nanocrystals grown by a solvothermal method. Average and local structures were refined by combining Rietveld and PDF analysis. We found that a rhombohedrally distorted NbO$$_6$$ octahedron was maintained in short-range order region, even in the nanocrystals with a cubic average structure. The cubic structure of KNbO$$_3$$ nanocrystals were observed as a disordered phase of the rhombohedral structure. The disordered feature can be understood that the structural transformation owing to the particle-size effect is analogous to the temperature-driven phase transition.

論文

Synthesis of new perovskite-type oxyfluorides, BaInO$$_{2}$$F and comparison of the structure among perovskite-type oxyfluorides

勝又 哲裕*; 鈴木 涼*; 佐藤 直人*; 鈴木 俊平*; 中島 護*; 稲熊 宜之*; 森 大輔*; 相見 晃久*; 米田 安宏

Journal of Solid State Chemistry, 279, p.120919_1 - 120919_8, 2019/11

 被引用回数:1 パーセンタイル:100(Chemistry, Inorganic & Nuclear)

A new perovskite-type fluoride, BaInO$$_2$$F was synthesized and compared with other perovskite-type oxyfluorides. The atomic size of anions influences on the local structure and the average structure obtained from the refinement of the diffraction pattern is the cubic for most perovskite-type oxyfluorides.

論文

Electronic structure of UTe$$_2$$ studied by photoelectron spectroscopy

藤森 伸一; 川崎 郁斗; 竹田 幸治; 山上 浩志; 仲村 愛*; 本間 佳哉*; 青木 大*

Journal of the Physical Society of Japan, 88(10), p.103701_1 - 103701_5, 2019/10

 被引用回数:4 パーセンタイル:14.41(Physics, Multidisciplinary)

The electronic structure of the unconventional superconductor $$mathrm{UTe_2}$$ was studied by resonant photoelectron spectroscopy (RPES) and angle-resolved photoelectron spectroscopy (ARPES) with soft X-ray synchrotron radiation. The partial $$mathrm{U}~5f$$ density of states of $$mathrm{UTe_2}$$ were imaged by the $$mathrm{U}~4d$$ - $$5f$$ RPES and it was found that the $$mathrm{U}~5f$$ state has an itinerant character, but there exists an incoherent peak due to the strong electron correlation effects. Furthermore, an anomalous admixture of the $$mathrm{U}~5f$$ states into the $$mathrm{Te}~5p$$ bands was observed at a higher binding energy, which cannot be explained by band structure calculations. On the other hand, the band structure of $$mathrm{UTe_2}$$ was obtained by ARPES and its overall band structure were mostly explained by band structure calculations. These results suggest that the $$mathrm{U}~5f$$ states of $$mathrm{UTe_2}$$ have itinerant but strongly-correlated nature with enhanced hybridization with the $$mathrm{Te}~5p$$ states.

論文

Element-specific density of states of Co$$_{2}$$MnGe revealed by resonant photoelectron spectroscopy

河野 嵩*; 鹿子木 将明*; 吉川 智己*; Wang, X.*; 角田 一樹*; 宮本 幸治*; 室 隆桂之*; 竹田 幸治; 斎藤 祐児; 後藤 一希*; et al.

Physical Review B, 100(16), p.165120_1 - 165120_6, 2019/10

 被引用回数:0 パーセンタイル:100(Materials Science, Multidisciplinary)

Resonant photoelectron spectroscopy at the Co and Mn 2${it p}$ core absorption edges of half-metallic Co$$_{2}$$MnGe has been performed to determine the element-specific density of states (DOS). A significant contribution of the Mn 3${it d}$ partial DOS near the Fermi level ($$E_{F}$$) was clarified by measurement at the Mn 2${it p}$ absorption edge. Further analysis by first-principles calculation revealed that it has $$t_{2g}$$ symmetry, which must be responsible for the electrical conductivity along the line perpendicular to the film plane. The dominant normal Auger contribution observed at the Co 2${it p}$ absorption edge indicates delocalization of photoexcited Co 3${it d}$ electrons. The difference in the degrees of localization of the Mn 3${it d}$ and Co 3${it d}$ electrons in Co$$_{2}$$MnGe is explained by the first-principles calculation.

論文

Magnetic-impurity-induced modifications to ultrafast carrier dynamics in the ferromagnetic topological insulators Sb$$_{2-x}$$V$$_{x}$$Te$$_{3}$$

角田 一樹*; 鹿子木 将明*; Reimann, J.*; Nurmamat, M.*; 後藤 伸一*; 竹田 幸治; 斎藤 祐児; Kokh, K. A.*; Tereshchenko, O. E.*; G$"u$dde, J.*; et al.

New Journal of Physics (Internet), 21(9), p.093006_1 - 093006_8, 2019/09

 被引用回数:1 パーセンタイル:50.85(Physics, Multidisciplinary)

We systematically investigate the magnetic, structural and electronic properties and the ultrafast carrier dynamics in a series of V-doped Sb$$_{2}$$Te$$_{3}$$ samples of composition Sb$$_{2-x}$$V$$_{x}$$Te$$_{3}$$ with x = 0, 0.015 and 0.03. Element specific X-ray magnetic circular dichroism signifies that the ferromagnetism of V-doped Sb$$_{2}$$Te$$_{3}$$ is governed by the p-d hybridization between the host carrier and the magnetic dopant. Time- and angle-resolved photoemission spectroscopy has revealed that the V impurity induced states underlying the topological surface state (TSS) add scattering channels that significantly shorten the duration of transient surface electrons down to 100 fs scale. This is in a sharp contrast to the prolonged duration reported for pristine samples though the TSS is located inside the bulk energy gap of the host in either magnetic or non-magnetic cases. It implies the presence of a mobility gap in the bulk energy gap region of the host material.

論文

ペロフスカイト型酸フッ化物における許容因子と結晶構造との関係

勝又 哲裕*; 稲熊 宣之*; 森 大輔*; 相見 晃久*; 米田 安宏

セラミックス, 54(9), p.629 - 632, 2019/09

ABO$$_3$$型ペロフスカイトフッ化物の結晶構造解析を放射光高エネルギーX線回折を用いて行った。ペロフスカイト型フッ化物においては許容因子の影響は局所構造に反映され、従来型の周期的構造を仮定した結晶構造解析においては平均構造は立方晶となることがわかった。

論文

放射光リアルタイム光電子分光で観る半導体表面の酸素分子の吸着反応

吉越 章隆

放射光, 32(4), p.185 - 198, 2019/07

放射光軟X線光電子分光は、固体表面の化学状態の精密分析に適した手法である。SPring-8の軟X線放射光を使うと気体孤立分子の固体表面との間で起きる化学反応を実時間"その場"観察する放射光リアルタイム光電子分光が可能となる。酸素分子による表面酸化は、半導体絶縁膜の形成などの表面機能化や燃料電池の電極反応、三元触媒反応や錆(腐食現象)などナノテクノロジー, 環境・エネルギー, 物質・材料のさまざまな研究分野に関係する重要な反応である。本稿では、シリコン単結晶の表面酸化における酸素吸着反応に焦点を当てる。著者が進めてきた一連の研究の紹介を通して、固体表面における分子吸着反応研究の重要性とそのメカニズム解明あるいは新規反応探索に対する放射光リアルタイム光電子分光の有用性を述べるとともに将来展望を試みた。

論文

Proton chelating ligands drive improved chemical separations for rhodium

成田 弘一*; Nicolson, R. M.*; 元川 竜平; 伊藤 文之*; 森作 員子*; 後藤 みどり*; 田中 幹也*; Heller, W. T.*; 塩飽 秀啓; 矢板 毅; et al.

Inorganic Chemistry, 58(13), p.8720 - 8734, 2019/07

 被引用回数:0 パーセンタイル:100(Chemistry, Inorganic & Nuclear)

Current industrial practices to extract rhodium from virgin ores carry a heavy environmental burden. Improving the efficiency of the hydrometallurgical processes to separate and recover rhodium from other precious metals provides an opportunity to improve the materials and energy balances, but the presence of mixed chloride-rhodium species following leaching by acid chloride media complicates the recovery process. In this work we have applied a broad range of analytical techniques (FT-IR spectroscopy, X-ray diffraction, EXAFS, water-transfer analysis, small-angle neutron scattering, NMR spectroscopy, and electrospray mass spectrometry), which together show that the amino-amide reagent preferentially transports chlorido-rhodium species as a 1:2 neutral assembly from aqueous 2.0 M HCl phase into an organic phase. The extractants then ligate in the outer coordination shell of the chloride-rhodium anion, making this an efficient separation process. In this study, we found that protonation to the extractants induced to form a proton chelate ring, which pre-organises the ligand to present an array of charge diffuse C-H bonds. This templated arrangement of positive dipoles favors complexation to the charge diffuse chloride-rhodium anion over the more charge-dense chloride anion.

論文

Electronic structure of the high-$$T_C$$ ferromagnetic semiconductor (Ga,Fe)Sb; X-ray magnetic circular dichroism and resonance photoemission spectroscopy studies

坂本 祥哉*; Tu, N. T.*; 竹田 幸治; 藤森 伸一; Hai, P. N.*; Anh, L. D.*; 若林 勇希*; 芝田 悟朗*; 堀尾 眞史*; 池田 啓祐*; et al.

Physical Review B, 100(3), p.035204_1 - 035204_8, 2019/07

The electronic structure and the magnetism of the ferromagnetic semiconductor (Ga,Fe)Sb, whose Curie temperature $$T_{rm C}$$ can exceed room temperature, were investigated by means of X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichroism (XMCD), and resonance photoemission spectroscopy (RPES). The line-shape analyses of the XAS and XMCD spectra suggest that the ferromagnetism is of intrinsic origin. The orbital magnetic moments deduced using XMCD sum rules were found to be large, indicating that there is a considerable 3$$d^{6}$$ contribution to the ground state of Fe. From RPES, we observed a strong dispersive Auger peak and nondispersive resonantly enhanced peaks in the valence-band spectra. The latter is a fingerprint of the correlated nature of Fe 3$$d$$ electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3$$d$$ states have a finite contribution to the density of states at the Fermi energy. These states, presumably consisting of majority-spin $$p$$-$$d$$ hybridized states or minority-spin e states, would be responsible for the ferromagnetic order in this material.

論文

Electronic structure of the high-T$$_{C}$$ ferromagnetic semiconductor (Ga,Fe)Sb; X-ray magnetic circular dichroism and resonance photoemission spectroscopy studies

坂本 祥哉*; Tu, N. T.*; 竹田 幸治; 藤森 伸一; Hai, P. N.*; Anh, L. D.*; 若林 勇希*; 芝田 悟朗*; 堀尾 眞史*; 池田 啓祐*; et al.

Physical Review B, 100(3), p.035204_1 - 035204_8, 2019/07

 被引用回数:4 パーセンタイル:18.88(Materials Science, Multidisciplinary)

The electronic structure and the magnetism of the ferromagnetic semiconductor (Ga,Fe)Sb, whose Curie temperature $$T_{rm C}$$ can exceed room temperature, were investigated by means of X-ray absorption spectroscopy (XAS), X-ray magnetic circular dichroism (XMCD), and resonance photoemission spectroscopy (RPES). The line-shape analyses of the XAS and XMCD spectra suggest that the ferromagnetism is of intrinsic origin. The orbital magnetic moments deduced using XMCD sum rules were found to be large, indicating that there is a considerable 3$$d^{6}$$ contribution to the ground state of Fe. From RPES, we observed a strong dispersive Auger peak and nondispersive resonantly enhanced peaks in the valence-band spectra. The latter is a fingerprint of the correlated nature of Fe 3$$d$$ electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3$$d$$ states have a finite contribution to the density of states at the Fermi energy. These states would be responsible for the ferromagnetic order in this material.

論文

Mass transport in the PdCu phase structures during hydrogen adsorption and absorption studied by XPS under hydrogen atmosphere

Tang, J.*; 山本 達*; 小板谷 貴典*; 吉越 章隆; 徳永 拓馬*; 向井 孝三*; 松田 巌*; 吉信 淳*

Applied Surface Science, 480, p.419 - 426, 2019/06

 被引用回数:1 パーセンタイル:60.62(Chemistry, Physical)

他のPd合金よりも水素拡散係数が高く経済的に低コストなPdCu合金の水素吸着および吸収プロセス中の物質移動を調べた。この研究では、bcc構造の規則相(B2相)とfcc構造およびB2構造の混合相との比較が行われた。放射光を用いたその場超高真空X線光電子分光法および雰囲気X線光電子分光法を実施し、温度に対するPdおよびCu原子の化学状態を追跡した。初期吸着過程と吸収過程は2相で類似していたが、バルクへの水素拡散速度は混合相よりも規則相の方が高かった。水素吸着/吸収過程におけるPdとCu原子のダイナミクスは温度に大きく依存した。水素雰囲気では、Pd原子は373Kより下では表面偏析し、Cu原子は373Kより上で表面偏析した。本結果は理論計算とよく一致し水素透過材料の開発に向けた有益な情報となる。

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