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Observation of adsorbed hydrogen species on supported metal catalysts by inelastic neutron scattering

吉田 寿雄*; 山本 旭*; 細川 三郎*; 山添 誠司*; 吉川 聡一*; 原 賢二*; 中村 充孝; 蒲沢 和也*; 田中 庸裕*

Topics in Catalysis, 64(9-12), p.660 - 671, 2021/08

 被引用回数:0 パーセンタイル:0.01(Chemistry, Applied)

Inelastic neutron scattering (INS) enables direct and selective observation of H species due to the extremely large incoherent neutron scattering cross section of a hydrogen atom. In the present study, the adsorbed H species on some heterogeneous precious metal catalysts supported by alumina and carbon black were investigated by in situ INS spectroscopy with a newly designed sample cell. Three alumina-supported metal catalysts having Pt, Pd, and Rh metal nanoparticles with different particle sizes exhibited different INS spectra in intensities and band distribution. Observation of the H species on the metal nanoparticles and the alumina surface revealed their properties. In addition, the H atoms stored in Pd nanoparticles were observed as palladium hydride. In contrast, the H species on a Pt catalyst supported by carbon black were found to be strongly adsorbed on the carbon support.


Detection of hydroxyl and hydride functional groups in a ceria crystal under hydrogen reduction

松川 健*; 飯田 一樹*; 中村 充孝; 石垣 徹*

CrystEngComm (Internet), 23(12), p.2355 - 2359, 2021/03

 被引用回数:1 パーセンタイル:81.7(Chemistry, Multidisciplinary)

Neutron powder diffraction analysis revealed that ceria transformed into the oxyhydroxide structure by hydrogen treatment. Due to detection of the vibrational modes of both OH and CeH functional groups by inelastic neutron scattering measurements, the CeH functional group was revealed to possibly exist in ceria as an aperiodic structure.


Mode distribution analysis for superionic melt of CuI by coherent quasielastic neutron scattering

川北 至信; 菊地 龍弥*; 田原 周太*; 中村 充孝; 稲村 泰弘; 丸山 健二*; 山内 康弘*; 河村 聖子; 中島 健次

JPS Conference Proceedings (Internet), 33, p.011071_1 - 011071_6, 2021/03



Magnetic excitations of Sr$$_{3}$$Ir$$_{2}$$O$$_{7}$$ observed by inelastic neutron scattering technique

藤田 全基*; 池内 和彦*; 梶本 亮一; 中村 充孝

Journal of the Physical Society of Japan, 90(2), p.025001_1 - 025001_2, 2021/02

 被引用回数:0 パーセンタイル:0.01(Physics, Multidisciplinary)

In this short note, we report on the first inelastic neutron scattering (INS) study on high-energy magnetic excitations in Sr$$_{3}$$Ir$$_{2}$$O$$_{7}$$. We observed excitations between $$sim$$80 meV and $$sim$$180 meV. The peak position of the excitations is consistent with the dispersion of a single magnon determined by resonant inelastic X-ray scattering (RIXS) measurement. Thus, our results demonstrate the feasibility of INS for iridates, which has a large neutron absorption cross-section.


Identification of hydrogen species on Pt/Al$$_{2}$$O$$_{3}$$ by ${it in situ}$ inelastic neutron scattering and their reactivity with ethylene

山添 誠司*; 山本 旭*; 細川 三郎*; 福田 良一*; 原 賢二*; 中村 充孝; 蒲沢 和也*; 佃 達哉*; 吉田 寿雄*; 田中 庸裕*

Catalysis Science & Technology, 11(1), p.116 - 123, 2021/01

 被引用回数:2 パーセンタイル:66.59(Chemistry, Physical)

Hydrogen (H) species adsorbed on catalyst surfaces are key intermediates in catalytic hydrogenation reactions over supported metal catalysts. However, individual identification of H species on the metal catalysts has not been established to date. Here, we elucidated the H species on Pt/Al$$_{2}$$O$$_{3}$$ by the combination of ${it in situ}$ inelastic neutron scattering (INS) and density functional theory (DFT). Several H species in the presence of H$$_{2}$$ were successfully identified at different sites on the Pt surface and Al$$_{2}$$O$$_{3}$$ support. The ${it in situ}$ INS and FT-IR measurements revealed that the hydride/atop Pt-H, bridged perimeter/terrace Pt-H-Pt, and threefold Pt$$_{3}$$-H are active intermediates in the C$$_{2}$$H$$_{4}$$ hydrogenation reaction, whereas the edge Pt-H-Pt is a rather inert species. In addition, the ${it in situ}$ measurements indicate that the Al$$_{2}$$O$$_{3}$$ itself acts as hydrogen storage material by mediating AlO-H and Al-H-Al species, which serve H species in the C$$_{2}$$H$$_{4}$$ hydrogenation reaction.


Temporally decoherent and spatially coherent vibrations in metal halide perovskites

Zhang, D.*; Hu, X.*; Chen, T.*; Abernathy, D. L.*; 梶本 亮一; 中村 充孝; 古府 麻衣子; Foley, B. J.*; Yoon, M.*; Choi, J. J.*; et al.

Physical Review B, 102(22), p.224310_1 - 224310_10, 2020/12

 被引用回数:1 パーセンタイル:27.27(Materials Science, Multidisciplinary)

The long carrier lifetime and defect tolerance in metal halide perovskites (MHPs) are major contributors to the superb performance of MHP optoelectronic devices. Large polarons were reported to be responsible for the long carrier lifetime. Yet microscopic mechanisms of the large polaron formation, including the so-called phonon melting, are still under debate. Here, time-of-flight inelastic neutron scattering experiments and first-principles density-functional theory calculations were employed to investigate the lattice vibrations (or phonon dynamics) in methylammonium lead iodide, a prototypical example of MHPs. Our findings are that optical phonons lose temporal coherence gradually with increasing temperature which vanishes at the orthorhombic-to-tetragonal structural phase transition. Surprisingly, however, we found that the spatial coherence is still retained throughout the decoherence process. We argue that the temporally decoherent and spatially coherent vibrations contribute to the formation of large polarons in this metal halide perovskite.


Energy resolution and neutron flux of the 4SEASONS spectrometer revisited

梶本 亮一; 中村 充孝; 飯田 一樹*; 蒲沢 和也*; 池内 和彦*; 稲村 泰弘; 石角 元志*

Journal of Neutron Research, 22(2-3), p.99 - 107, 2020/10

The elastic energy resolution, integrated intensity, and peak intensity of the direct-geometry neutron chopper spectrometer 4SEASONS at Japan Proton Accelerator Research Complex (J-PARC) were re-investigated. This was done with respect to the incident energy and the rotation speed of the Fermi chopper using incoherent scattering of vanadium and simple analytical formulas. The model calculations reproduced the observed values satisfactorily. The present work should be useful for estimating in instrument performance in experiments.


Spin dynamics of a magnetic Weyl semimetal Sr$$_{1-x}$$Mn$$_{1-y}$$Sb$$_{2}$$

Cai, Z.*; Bao, S.*; Wang, W.*; Ma, Z.*; Dong, Z.-Y.*; Shangguan, Y.*; Wang, J.*; Ran, K.*; Li, S.*; 蒲沢 和也*; et al.

Physical Review B, 101(13), p.134408_1 - 134408_10, 2020/04

 被引用回数:1 パーセンタイル:27.27(Materials Science, Multidisciplinary)



Emergent spin-1 Haldane gap and ferroelectricity in a frustrated spin-$$frac{1}{2}$$ 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:2 パーセンタイル:47.94(Materials Science, Multidisciplinary)

We report experimental and theoretical evidence that Rb$$_2$$Cu$$_2$$Mo$$_3$$O$$_{12}$$ has a nonmagnetic tetramer ground state of a two-leg ladder comprising antiferromagnetically coupled frustrated spin-$$frac{1}{2}$$ 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.


The $$f$$-electron state of the heavy fermion superconductor NpPd$$_5$$Al$$_2$$ 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



Q dependence of magnetic resonance mode on FeTe$$_{0.5}$$Se$$_{0.5}$$ studied by inelastic neutron scattering

石角 元志*; 樹神 克明; 梶本 亮一; 中村 充孝; 稲村 泰弘; 池内 和彦*; Ji, S.*; 新井 正敏*; 社本 真一

Condensed Matter (Internet), 4(3), p.69_1 - 69_10, 2019/09



Applicability and limitations of $$G(r,E)$$ analysis transformed from the inelastic neutron scattering data

中村 充孝; 菊地 龍弥*; 川北 至信

Physica B; Condensed Matter, 567, p.61 - 64, 2019/08


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

最近、非弾性中性子散乱実験(INS)データから変換した実空間動的構造因子$$G(r,E)$$を用いた多結晶NaIのフォノンダイナミクスに関する研究報告を行った。この研究は、通常のINS実験条件(Q$$_{max} sim$$ 5$AA$^{-1}$$)であっても、物理的に十分意味のある実空間ダイナミクス情報が得られることを示したものであり、これまでに蓄積されてきた大量のINSデータの再利用と新たな視点での研究推進を促すものである。今回の発表では、$$G(r,E)$$解析の適用可能性とその限界について詳しく議論する。


Background issues encountered by cold-neutron chopper spectrometer AMATERAS

菊地 龍弥*; 中島 健次; 河村 聖子; 稲村 泰弘; 中村 充孝; 若井 大介*; 青山 和弘*; 岩橋 孝明*; 神原 理*

Physica B; Condensed Matter, 564, p.45 - 53, 2019/07

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

AMATERASはJ-PARC物質・生命科学実験施設に設置された冷中性子チョッパー型分光器である。この9年に亘る運用の中で得られたバッググラウンド(意図せずにデータ収集系に集積されるシグナル)についての知見をまとめた。それらは、ビームライン上にある物質から発生するガンマ線、ビームライン上にある機器から発生するブラッグ反射, 空気散乱, 電気ノイズ, 宇宙線などである。それらについてまとめると共に今後の可能な対策について述べる。これらは、同種の分光器にとっても役立つ情報となると期待する。


Status of neutron spectrometers at J-PARC

梶本 亮一; 横尾 哲也*; 中村 充孝; 川北 至信; 松浦 直人*; 遠藤 仁*; 瀬戸 秀紀*; 伊藤 晋一*; 中島 健次; 河村 聖子

Physica B; Condensed Matter, 562, p.148 - 154, 2019/06


 被引用回数:5 パーセンタイル:50.07(Physics, Condensed Matter)

Seven time-of-flight quasielastic/inelastic neutron scattering instruments are installed on six beamlines in the Materials and Life Science Experimental Facility (MLF) at the Japan Proton Accelerator Research Complex (JPARC). Four of these instruments are chopper-type direct-geometry spectrometers, one is a near-backscattering indirect-geometry spectrometer, and the other two are spin-echo-type spectrometers. This paper reviews the characteristic features, recent scientific outcomes, and progress in development of MLF spectrometers.


Quantum dynamics of hydrogen in the iron-based superconductor LaFeAsO$$_{0.9}$$D$$_{0.1}$$ measured with inelastic neutron spectroscopy

山浦 淳一*; 平賀 晴弘*; 飯村 壮史*; 村場 善行*; Bang, J.*; 池内 和彦*; 中村 充孝; 稲村 泰弘; 本田 孝志*; 平石 雅俊*; et al.

Physical Review B, 99(22), p.220505_1 - 220505_6, 2019/06

 被引用回数:1 パーセンタイル:11.39(Materials Science, Multidisciplinary)



Study on use of superconducting magnet and first inelastic neutron scattering experiment under magnetic field at 4SEASONS spectrometer

梶本 亮一; 石角 元志*; 吉良 弘*; 金子 耕士; 中村 充孝; 蒲沢 和也*; 稲村 泰弘; 池内 和彦*; 飯田 一樹*; 村井 直樹; et al.

Physica B; Condensed Matter, 556, p.26 - 30, 2019/03


 被引用回数:2 パーセンタイル:23.12(Physics, Condensed Matter)

Magnets are important for studying magnetism and are commonly used as sample environment devices of neutron scattering instruments. However, the use of magnets was prevented at the time-of-flight direct-geometry neutron spectrometer 4SEASONS in Materials and Life Science Experimental Facility (MLF) at J-PARC, because the instrument is surrounded by iron components, and it is equipped with a piece of equipment operated with magnetic bearings. In the present work, we investigate the influence of stray magnetic fields from a superconducting magnet which is shared among neutron scattering instruments in MLF. Based on the investigation, we modified 4SEASONS such that it can be used with the magnet. Finally, we successfully performed the first inelastic neutron scattering experiments with applied magnetic fields using this sample environment.


Performances of oscillating radial collimator for the Fermi chopper spectrometer 4SEASONS at J-PARC

中村 充孝; 神原 理*; 飯田 一樹*; 梶本 亮一; 蒲沢 和也*; 池内 和彦*; 石角 元志*; 青山 和弘*

Physica B; Condensed Matter, 551, p.480 - 483, 2018/12


 被引用回数:1 パーセンタイル:8.47(Physics, Condensed Matter)



Phonon dynamics of NaI investigated by G($$r,E$$) analysis

中村 充孝; 菊地 龍弥*; 蒲沢 和也*; 川北 至信

Physica B; Condensed Matter, 551, p.351 - 354, 2018/12


 被引用回数:2 パーセンタイル:17.02(Physics, Condensed Matter)



Anomaly of structural relaxation in complex liquid metal of bismuth; Dynamic correlation function of coherent quasi-elastic neutron scattering

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:7 パーセンタイル:49.86(Physics, Condensed Matter)



Gapless magnetic excitation in a heavily electron-doped antiferromagnetic phase of LaFeAsO$$_{0.5}$$D$$_{0.5}$$

玉造 博夢*; 平賀 晴弘*; 池内 和彦*; 飯村 壮史*; 村場 善行*; 中村 充孝; 佐賀山 基*; 山浦 淳一*; 村上 洋一*; 倉本 義夫*; et al.

Physical Review B, 98(17), p.174415_1 - 174415_6, 2018/11


 被引用回数:2 パーセンタイル:17.02(Materials Science, Multidisciplinary)


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