Electrocatalytic nitrous oxide reduction reaction at Sn-modified Pd-Pt single crystalline electrodes in acidic media

加藤 優*; Zheng, J.*; Deng, Y.*; 斎藤 史恵*; 鵜沼 佑規*; 岡 紗雪*; 田村 和久; 八木 一三*

ACS Catalysis, 15(10), p.7710 - 7719, 2025/04

https://doi.org/10.1021/acscatal.5c00379

Nitrous oxide (NO) is a greenhouse and an ozone-depleting gas. Electrocatalytic NO reduction reaction (NORR) is known to be catalyzed at noble metal electrodes such as Pd and Pt, and the surface modification of such noble metals with Sn is known to increase the NORR in acidic media. However, the role of Sn at the surface remains unclear. In this work, NORR activity was investigated for single-crystalline Pt, Pd, and Pd-Pt electrodes with the (111) or (100) plane in the presence and absence of Sn at the electrode surface in acidic media. In situ X-ray crystal truncation rod (CTR) measurements of Sn-modified Pt(111) and Pd(111) electrodes revealed the presence of metallic Sn and SnO at their surfaces. The surface Sn modification enhances the NORR activity for Pd-Pt(100) or Pd(100) electrodes but not for the Pt(111), Pd-Pt(111), or Pt(100) electrodes.

A Systematic approach for the adequacy analysis of a set of experimental databases; Application in the framework of the ATRIUM activity

Baccou, J.*; Glantz, T.*; Ghione, A.*; Sargentini, L.*; Fillion, P.*; Damblin, G.*; Sueur, R.*; Iooss, B.*; Fang, J.*; Liu, J.*; et al.

Nuclear Engineering and Design, 421, p.113035_1 - 113035_16, 2024/05

https://doi.org/10.1016/j.nucengdes.2024.113035

In the Best-Estimate Plus Uncertainty (BEPU) framework, the use of best-estimate code requires to go through a Verification, Validation and Uncertainty Quantification process (VVUQ). The relevance of the experimental data in relation to the physical phenomena of interest in the VVUQ process is crucial. Adequacy analysis of selected experimental databases addresses this problem. The outcomes of the analysis can be used to select a subset of relevant experimental data, to encourage designing new experiments or to drop some experiments from a database because of their substantial lack of adequacy. The development of a specific transparent and reproducible approach to analyze the relevance of experimental data for VVUQ still remains open and is the topic of this contribution. In this paper, the concept of adequacy initially introduced in the OECD/NEA SAPIUM (Systematic APproach for model Input Uncertainty quantification Methodology) activity is formalized. It is defined through two key properties, called representativeness and completeness, that allows considering the multifactorial dimension of the adequacy problem. A new systematic approach is then proposed to analyze the adequacy of a set of experimental databases. It relies on the introduction of two sets of criteria to characterize representativeness and completeness and on the use of multi-criteria decision analysis method to perform the analysis. Finally, the approach is applied in the framework of the new OECD/NEA ATRIUM activity which includes a set of practical IUQ exercises in thermal-hydraulics to test the SAPIUM guideline in determining input uncertainties and forward propagating them on an application case. It allows evaluating the adequacy of eight experimental databases coming from the Super Moby-dick, Sozzi-Sutherland and Marviken experiments and identifying the most adequate ones.

垂直磁気異方性を示す鉄挿入遷移金属ダイカルコゲナイドFeTaSのX線磁気円二色性による研究; FeTiSとの比較

芝田 悟朗; Won, C.*; Kim, J.*; 野中 洋亮*; 池田 啓祐*; Wan, Y.*; 鈴木 雅弘*; 小出 常晴*; 田中 新*; Cheong, S.-W.*; et al.

Photon Factory Activity Report 2022 (インターネット), 2 Pages, 2023/00

https://pfwww.kek.jp/acr/2022pdf/u_reports.html

Feをインターカレートした遷移金属ダイカルコゲナイド化合物FeTiSおよびFeTaSは、巨大な保磁力および垂直磁気異方性を示す強磁性体になることが知られている。我々は以前、FeTiSについてのX線磁気円二色性(XMCD)実験の結果から、Feの凍結していない軌道磁気モーメントが結晶場の1次摂動によって直接磁気異方性エネルギーを生むことを明らかにした。今回、FeTiSよりもさらに強い磁気異方性を示す遷移金属ダイカルコゲナイドFeTaSについて同様にXMCD実験を行い、磁気異方性の強さが何によって左右されているかを探ることを試みた。

Paramagnetic spin Hall magnetoresistance

大柳 洸一*; Gomez-Perez, J. M.*; Zhang, X.-P.*; 吉川 貴史*; Chen, Y.*; Sagasta, E.*; Chuvilin, A.*; Hueso, L. E.*; Golovach, V. N.*; Sebastian Bergeret, F.*; et al.

Physical Review B, 104(13), p.134428_1 - 134428_14, 2021/10

https://doi.org/10.1103/PhysRevB.104.134428

We report the observation of the spin Hall magnetoresistance (SMR) in a paramagnetic insulator. By measuring the transverse resistance in a Pt/GdGaO (GGG) system at low temperatures, paramagnetic SMR is found to appear with an intensity that increases with the magnetic field aligning GGG's spins. The observed effect is well supported by a microscopic SMR theory, which provides the parameters governing the spin transport at the interface. Our findings clarify the mechanism of spin exchange at a Pt/GGG interface, and demonstrate tunable spin-transfer torque through the field-induced magnetization of GGG. In this regard, paramagnetic insulators offer a key property for future spintronic devices.

Triplon current generation in solids

Chen, Y.*; 佐藤 正寛*; Tang, Y.*; 塩見 雄毅*; 大柳 洸一*; 益田 隆嗣*; 南部 雄亮*; 藤田 全基*; 齊藤 英治

Nature Communications (Internet), 12, p.5199_1 - 5199_7, 2021/08

https://doi.org/10.1038/s41467-021-25494-7

A triplon refers to a fictitious particle that carries angular momentum corresponding to the elementary excitation in a broad class of quantum dimerized spin systems. Such systems without magnetic order have long been studied as a testing ground for quantum properties of spins. Although triplons have been found to play a central role in thermal and magnetic properties in dimerized magnets with singlet correlation, a spin angular momentum flow carried by triplons, a triplon current, has not been detected yet. Here we report spin Seebeck effects induced by a triplon current: triplon spin Seebeck effect, using a spin-Peierls system CuGeO. The result shows that the heating-driven triplon transport induces spin current whose sign is positive, opposite to the spin-wave cases in magnets. The triplon spin Seebeck effect persists far below the spin-Peierls transition temperature, being consistent with a theoretical calculation for triplon spin Seebeck effects.

Quasifree neutron knockout reaction reveals a small -Orbital component in the Borromean nucleus B

Yang, Z. H.*; 久保田 悠樹*; Corsi, A.*; 吉田 数貴; Sun, X.-X.*; Li, J. G.*; 木村 真明*; Michel, N.*; 緒方 一介*; Yuan, C. X.*; et al.

Physical Review Letters, 126(8), p.082501_1 - 082501_8, 2021/02

AA2020-0819.pdf:1.29MB

https://doi.org/10.1103/PhysRevLett.126.082501

ボロミアン核であり中性子ハロー構造が期待されるBに対する(,)反応実験を行った。断面積の運動量分布を分析することで、と軌道の分光学的因子を決定した。驚くべきことに、の分光学的因子は9(2)%と小さいことが明らかになった。この結果は、連続状態を含むdeformed relativistic Hartree-Bogoliubov理論によってよく説明された。本研究の結果によると、現在知られているハロー構造を持つとされる原子核の中でBはおよび軌道の成分が最も小さく、または軌道成分が支配的であることが必ずしもハロー構造の前提条件ではない可能性を示唆している。

Surface coverage dependence of spin-to-charge current across Pt/MoS/YFeO layers via longitudinal spin Seebeck effect

Lee, W.-Y.*; Park, N.-W.*; Kang, M.-S.*; Kim, G.-S.*; Jang, H. W.*; 齊藤 英治; Lee, S.-K.*

Journal of Physical Chemistry Letters (Internet), 11(13), p.5338 - 5344, 2020/07

https://doi.org/10.1021/acs.jpclett.0c01502

The voltage induced by the inverse spin Hall effect (ISHE) is affected by several factors, including the spin Hall angle of the normal metal (NM), the quality and magnetic properties of the ferromagnetic material (FM), and the interface conditions between the NM and FM bilayers in longitudinal spin Seebeck effect (LSSE) measurement. Specifically, the interface conditions in NM/FM systems via LSSE devices play a crucial role in determining the efficiency of spin current injection into the NM layer. In this letter, we report a new approach to controlling the efficiency of spin current injection into a Pt layer across a Pt/YFeO (YIG) interface by surface coverage of the intermediate layer. A continuous, large-area multilayer molybdenum dichalcogenide (MoS) thin film grown by chemical vapor deposition is inserted between the Pt and YIG layers in the LSSE configuration. We found that, when the large-area multilayer MoS film was present, the measured ISHE-induced voltage and theoretically calculated spin current in the Pt/MoS/YIG trilayer increased by 510% and 470%, respectively, compared to those of a Pt/YIG bilayer. The induced voltage and spin current were very sensitive to the surface conductance, which was affected by the surface coverage of the multilayer MoS films in the LSSE measurement. Furthermore, the theoretically calculated spin current and spin mixing conductance in the trilayer geometry are in qualitatively good agreement with the experimental observations. These measurements enable us to explain the effect of the interface conditions on the spin Seebeck effect in spin transport.

Crystalline dependence of spin transmission in CrO thin films

Qin, J.*; Hou, D.*; Chen, Y.*; 齊藤 英治; Jin, X.*

Journal of Magnetism and Magnetic Materials, 501, p.166362_1 - 166362_4, 2020/05

https://doi.org/10.1016/j.jmmm.2019.166362

Spin transmission in CrO films of different crystalline textures is studied experimentally. With YFeO/CrO/Pt trilayer devices, a spin current is injected into CrO by spin pumping from YFeO, and the spin transmission is monitored by the inverse spin Hall voltage () in Pt. For (0001) plane textured CrO films, vanishes quickly below the Nel temperature. However, the shows a broad shoulder below the Nel temperature for and plane co-textured CrO. Such a difference in the temperature dependence of CrO can be understood by the different Nel vector orientations with respect to the injected spin moment direction.

Spin Seebeck mechanical force

針井 一哉; Seo, Y.-J.*; 堤 康雅*; 中堂 博之; 大柳 洸一*; 松尾 衛; 塩見 雄毅*; 小野 崇人*; 前川 禎通; 齊藤 英治

Nature Communications (Internet), 10, p.2616_1 - 2616_5, 2019/06

https://doi.org/10.1038/s41467-019-10625-y

Electric current has been used to send electricity to far distant places. On the other hand, spin current, a flow of electron spin, can in principle also send angular momentum to distant places. In a magnet, there is a universal spin carrier called a spin wave, a wave-type excitation of magnetization. Since spin waves exhibit a long propagation length, it should be able to send angular momentum that can generate torque and force at a distant place: a new function of magnets. Here we observe mechanical angular momentum transmission and force generation due to spin waves injected into YFeO by the spin-Seebeck effect. The spin-wave current, transmitted through a YFeO micro cantilever, was found to create a mechanical force on the cantilever as a non-local reaction of the spin-Seebeck effect. Spin-wave current can be generated remotely even in open circuits, and it can be used to drive micro mechanical devices.

Negative Te spin polarization responsible for ferromagnetic order in the doped topological insulator V(SbBi)Te

Ye, M.*; Xu, T.*; Li, G.*; Qiao, S.*; 竹田 幸治; 斎藤 祐児; Zhu, S.-Y.*; Nurmamat, M.*; 角田 一樹*; 石田 行章*; et al.

Physical Review B, 99(14), p.144413_1 - 144413_7, 2019/04

AA2018-0697.pdf:1.89MB

https://doi.org/10.1103/PhysRevB.99.144413

We investigate the microscopic origin of ferromagnetism coupled with topological insulators in V-doped (Sb,Bi)Te employing X-ray magnetic circular dichroism and angle-resolved two-photon photoemission spectroscopies, combined with first-principles calculations. We found an magnetic moment at the Te site anti-parallel to that of the V and Sb sites, which plays a key role in the ferromagnetic order. We ascribe it to the hybridization between Te 5 and V 3 majority spin states at the Fermi energy, consistent with the Zener-type - exchange interaction scenario. The substitution of Bi for Sb suppresses the bulk ferromagnetism by introducing extra electron carriers in the majority spin channel of the Te states that compensates the antiparallel magnetic moment on the Te site. Our findings reveal important clues to designing magnetic topological insulators with higher Curie temperature that work under ambient conditions.