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論文

Cu $$K$$-edge X-ray absorption fine structure study of $$T'$$-type $$RE$$$$_{2}$$CuO$$_{4+alpha-delta}$$ ($$RE$$ = Rare Earth); Toward unified understanding of electronic state of $$T'$$-type cuprate

Chen, Y.*; 浅野 駿*; Wang, T.*; Xie, P.*; 北山 慎之介*; 石井 賢司*; 松村 大樹; 辻 卓也; 谷口 貴紀*; 藤田 全基*

JPS Conference Proceedings (Internet), 38, p.011050_1 - 011050_6, 2023/05

https://doi.org/10.7566/JPSCP.38.011050

To investigate the variation of the electronic state of $$T'$$-type cuprate due to annealing, we performed Cu $$K$$-edge X-ray absorption fine structure measurements on Pr$$_{2}$$CuO$$_{4+alpha-delta}$$ (PCO) and Pr$$_{1.3}$$La$$_{0.7}$$CuO$$_{4+alpha-delta}$$ (PLCO). The induced electrons due to annealing ($$n_{AN}$$) in PCO and PLCO were approximately 2$$delta$$, consistent with a model of electron doping to Mott insulator. Here, $$alpha$$ and $$delta$$ represent the amount of excess oxygen from the stoichiometric composition in the as-sintered compound and that of oxygen loss due to annealing, respectively. Furthermore, the energy of the Einstein oscillator ($$hbaromega_{E}$$) for the Cu-O$$_{p}$$ bond was evaluated by extended X-ray absorption fine structure analysis. (O$$_{p}$$ denotes the in-plane oxygen.) We found a small annealing effect on $$hbaromega_{E}$$ for both PCO and PLCO.

論文

Investigation of hydrogen superoxide adsorption during ORR on Pt/C catalyst in acidic solution for PEFC by ${it in-situ}$ high energy resolution XAFS

山本 直生*; 松村 大樹; 萩原 悠人*; 田中 啓偉*; 長谷川 優太*; 石井 賢司*; 田中 裕久*

Journal of Power Sources, 557, p.232508_1 - 232508_10, 2023/02

https://doi.org/10.1016/j.jpowsour.2022.232508
 被引用回数：2 パーセンタイル：29.01(Chemistry, Physical)

Oxygen Reduction Reaction (ORR) is one of the key electrochemical reactions, especially in Polymer Electrolyte Fuel Cells (PEFCs). In this work, the reaction pathway and intermediate species such as molecular-type oxygen during ORR were discussed. High energy resolution X-ray absorption fine structure spectra at the Pt L$$_{3}$$-edge were obtained to observe the electronic structure of Pt catalyst. Carbon-supported Pt nanoparticles as powder catalysts were used for measurement as more realistic conditions, and the species adsorbed on the Pt nanoparticles were analyzed while controlling under the potentials in acidic electrolyte solution with N$$_{2}$$ or O$$_{2}$$ gas bubbling. Molecular-type oxygen adsorption species is observed only in the O$$_{2}$$-bubbled electrolyte solution. This intermediate adsorption species is assigned to a hydrogen superoxide.

論文

Distinct variation of electronic states due to annealing in $$T'$$-type La$$_{1.8}$$Eu$$_{0.2}$$CuO$$_{4}$$ and Nd$$_{2}$$CuO$$_{4}$$

浅野 駿*; 石井 賢司*; 松村 大樹; 辻 卓也; 工藤 康太*; 谷口 貴紀*; 齋藤 真*; 春原 稔樹*; 川股 隆行*; 小池 洋二*; et al.

Physical Review B, 104(21), p.214504_1 - 214504_7, 2021/12

https://doi.org/10.1103/PhysRevB.104.214504
 被引用回数：0 パーセンタイル：0(Materials Science, Multidisciplinary)

We performed Cu K-edge X-ray absorption fine-structure measurements on $$T'$$-type La$$_{1.8}$$Eu$$_{0.2}$$CuO$$_{4}$$ (LECO) and Nd$$_{2}$$CuO$$_{4}$$ (NCO) to investigate the variation in the electronic state associated with the emergence of superconductivity due to annealing. The X-ray absorption near-edge structure spectra of as-sintered (AS) LECO are quite similar to those of AS NCO, indicating that the ground state of AS LECO is a Mott insulator. The electron density after annealing $$n_{rm AN}$$ was evaluated for both superconducting LECO and nonsuperconducting NCO and was found to be 0.40 and 0.05 electron per Cu atom, respectively. In LECO but not in NCO, extended X-ray absorption fine-structure analysis revealed a reduction in the strength of the Cu-O bond in the CuO$$_{2}$$ plane due to annealing, which is consistent with the screening effect on phonons in the metallic state. The origin of the difference in doping processes due to annealing is discussed in relation to the size of the charge-transfer gap.

論文

Feasibility study of magnetic-domain observation by means of non-resonant magnetic X-ray diffraction

稲見 俊哉*; 菖蒲 敬久; 石井 賢司*

IEEE Transactions on Magnetics, 57(3, Part 2), p.6400105_1 - 6400105_5, 2021/03

https://doi.org/10.1109/TMAG.2020.3046006
 被引用回数：0 パーセンタイル：0(Engineering, Electrical & Electronic)

Although the observation of magnetic domains well below the surface of a sample appears to be relatively easy, in reality, magnetic domains inside metallic samples have not been investigated in detail due to a lack of adequate techniques. Non-resonant magnetic X-ray diffraction (NRMXRD) is a candidate for such 3-D magnetic microscopy. A relatively small focus size of less than 100 nm and a relatively long attenuation length of more than 100 $$mu$$m can be obtained by using high-energy synchrotron X-rays. However, NRMXRD has a disadvantage in that the magnetic contrast is low. It is known that the magnetic contrast in NRMXRD increases with increasing the total polarization of the incident X-rays. In this feasibility study, we carried out NRMXRD experiments on a metallic iron sample to examine whether the magnetic contrast can be sufficiently enhanced even for high-energy X-rays.

論文

Electrochemical adsorption on Pt nanoparticles in alkaline solution observed using in situ high energy resolution X-ray absorption spectroscopy

草野 翔吾*; 松村 大樹; 石井 賢司*; 田中 裕久*; 水木 純一郎*

Nanomaterials (Internet), 9(4), p.642_1 - 642_14, 2019/04

https://doi.org/10.3390/nano9040642
 被引用回数：7 パーセンタイル：37.59(Chemistry, Multidisciplinary)

The oxygen reduction reaction (ORR) on Pt/C in alkaline solution was studied by in situ high energy resolution X-ray absorption spectroscopy. To discuss the X-ray absorption near-edge structure (XANES), this paper introduced the rate of change of the $$Delta mu$$ (RCD), which is an analysis method that is sensitive to surface adsorption. The surface adsorptions as hydrogen (below 0.34 V), superoxide anion (from 0.34 V to 0.74 V), hydroxyl species (from 0.44 V to 0.74 V), atomic oxygen (above 0.74 V), and $$alpha$$-PtO$$_{2}$$ (above 0.94 V) were distinguished. It is clarified that the catalytic activity in an alkaline solution is enhanced by the stability of atomic oxygen and the low stability of superoxide anion/peroxide adsorption on the platinum surface.

論文

Ce substitution and reduction annealing effects on electronic states in Pr$$_{2-x}$$Ce$$_x$$CuO$$_4$$ studied by Cu $$K$$-edge X-ray absorption spectroscopy

浅野 駿*; 石井 賢司*; 松村 大樹; 辻 卓也; 伊奈 稔哲*; 鈴木 謙介*; 藤田 全基*

Journal of the Physical Society of Japan, 87(9), p.094710_1 - 094710_5, 2018/09

https://doi.org/10.7566/JPSJ.87.094710
 被引用回数：12 パーセンタイル：64.96(Physics, Multidisciplinary)

We investigated the Ce substitution and reduction annealing effects on the electronic states at copper sites by Cu $$K$$-edge X-ray absorption near-edge structure measurements in Pr$$_{2-x}$$Ce$$_x$$CuO$$_{4+alpha-delta}$$ (PCCO) with varying $$x$$ and $$delta$$ (amount of oxygen loss during annealing). Absorption near-edge spectra were modified by Ce substitution and reduction annealing similarly with increasing $$x$$ and $$delta$$. Considering electron doping by Ce substitution, this similarity indicates an increase in electron number at the copper sites due to annealing ($$n_{AN}$$). Furthermore, quantitative analyses of the spectra clarified that the number of Cu$$^+$$ sites, corresponding to the induced electron number by Ce substitution increases linearly with $$x$$ in the as-sintered PCCO, whereas $$n_{AN}$$ is not exactly equal to 2$$delta$$. For each $$x$$-fixed sample, $$n_{AN}$$tends to exceed 2$$delta$$ with increasing $$delta$$, suggesting the emergence of two types of carrier due to annealing.

論文

Pt, PtCo触媒表面の酸素吸着に及ぼす水の影響

Cui, Y.-T.*; 原田 慈久*; 丹羽 秀治*; 尾嶋 正治*; 畑中 達也*; 中村 直樹*; 安藤 雅樹*; 吉田 利彦*; 石井 賢司*; 松村 大樹

NanotechJapan Bulletin (インターネット), 11(4), 6 Pages, 2018/08

固体高分子形燃料電池の正極には白金ナノ粒子触媒が使用されているが、加湿によって活性化過電圧が発生して性能が低下することが知られている。この原因を解明し、低減する技術を確立することが、燃料電池の性能向上とコスト低減に向けた喫緊の課題となっている。しかしながら、従来の方法で測定した白金ナノ粒子触媒のX線吸収スペクトルでは、白金の内殻正孔の寿命によるスペクトル幅の広がりで微細な構造がぼやけてしまい、吸着に起因する電子状態の変化を捉えることが困難であった。そこで本研究では、非弾性X線散乱装置を利用した高分解能型の蛍光X線吸収分光法による測定を行った。結果、酸素が水と共存することにより、白金の酸化を促進することが明瞭に検出でき、実験的に初めて明らかにすることができた。本来、触媒である白金は反応前後で不変であるべきものであるが、この反応では、白金上で酸素が水と共吸着することにより安定化して反応の進行を遅らせた結果、過電圧がより大きく生じていると解釈できる。また、白金コバルト合金ナノ粒子についても調べたところ、酸素と水の共吸着による酸化促進効果がほとんど起こらないことを見出した。

論文

Reduction and oxidation annealing effects on Cu $$K$$-edge XAFS for electron-doped cuprate superconductors

浅野 駿*; 鈴木 謙介*; 松村 大樹; 石井 賢司*; 伊奈 稔哲*; 藤田 全基*

Journal of Physics; Conference Series, 969, p.012051_1 - 012051_5, 2018/04

https://doi.org/10.1088/1742-6596/969/1/012051
 被引用回数：3 パーセンタイル：82.15(Physics, Applied)

Reduction and oxidation annealing effects on the electronic states around the copper sites for Pr$$_{2-x}$$Ce$$_x$$CuO$$_4$$ and Nd$$_{2-x}$$Ce$$_x$$CuO$$_4$$ with $$x$$ = 0 and $$x$$ = 0.15 were investigated by Cu $$K$$-edge X-ray absorption measurements. Cu $$K$$ near-edge spectra were changed by the reduction annealing in a manner similar to the case of Ce substitution for both $$x$$ = 0 and $$x$$ = 0.15. This means an increase of electron density at the copper sites, indicating the aspect of electron doping in the reduction annealing. This reduction annealing effect on the near-edge spectra are reverted by the additional oxidation annealing. The amount of electron density around the copper sites is varied by the reduction and oxidation annealing, reversibly, corresponding to the reversible variation of the physical property from insulating to superconductivity.

論文

Observation of momentum-dependent charge excitations in hole-doped cuprates using resonant inelastic X-ray scattering at the oxygen $$K$$ edge

石井 賢司*; 遠山 貴巳*; 浅野 駿*; 佐藤 研太朗*; 藤田 全基*; 脇本 秀一; 筒井 健二*; 曽田 繁利*; 宮脇 淳*; 丹羽 秀治*; et al.

Physical Review B, 96(11), p.115148_1 - 115148_8, 2017/09

AA2017-0402.pdf:0.81MB

https://doi.org/10.1103/PhysRevB.96.115148
 被引用回数：29 パーセンタイル：77.9(Materials Science, Multidisciplinary)

We investigate electronic excitations in La$$_{2-x}$$(Br,Sr)$$_x$$CuO$$_4$$ using resonant inelastic X-ray scattering (RIXS) at the oxygen $$K$$ edge. We observed momentum-dependent spectral weight below 1 eV, which is consistent with theoretical calculation of the dynamical charge structure factor on oxygen orbitals in a three-band Hubbard model. Our results confirm that the momentum-dependent charge excitations exist on the order of the transfer energy ($$t$$), and the broad spectral line shape indicates damped and incoherent character of the charge excitations at the energy range in the doped Mott insulators.

論文

Wetting induced oxidation of Pt-based nano catalysts revealed by ${{it in situ}}$ high energy resolution X-ray absorption spectroscopy

Cui, Y.-T.*; 原田 慈久*; 丹羽 秀治*; 畑中 達也*; 中村 直樹*; 安藤 雅樹*; 吉田 稔彦*; 石井 賢司*; 松村 大樹; 陰地 宏*; et al.

Scientific Reports (Internet), 7(1), p.1482_1 - 1482_8, 2017/05

https://doi.org/10.1038/s41598-017-00639-1
 被引用回数：19 パーセンタイル：49.58(Multidisciplinary Sciences)

In situ high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD-XAS) was used to systematically evaluate interactions of H$$_{2}$$O and O$$_{2}$$ adsorbed on Pt and Pt$$_{3}$$Co nanoparticle catalysts in different particle sizes. The systematic increase in oxidation due to adsorption of different species (H$$_{2}$$O adsorption $$<$$ O$$_{2}$$ adsorption $$<$$ O$$_{2}$$ + H$$_{2}$$O coadsorption) suggests that cooperative behavior between O$$_{2}$$ and H$$_{2}$$O adsorptions is responsible for the overpotential induced by hydrated species in fuel cells. From the alloying and particle size effects, it is found that both strength of O$$_{2}$$/H$$_{2}$$O adsorption and their cooperative effect upon coadsorption are responsible for the specific activity of Pt catalysts.

論文

Electronic structure of Pt and Pt-Co nanoparticles with O$$_{2}$$ and O$$_{2}$$/H$$_{2}$$O adsorption revealed by in situ XAFS and hard X-ray photoelectron spectroscopy

Cui, Y.*; 原田 慈久*; 畑中 達也*; 中村 直樹*; 安藤 雅樹*; 吉田 稔彦*; 池永 英司*; 石井 賢司*; 松村 大樹; Li, R.*; et al.

ECS Transactions, 72(8), p.131 - 136, 2016/10

https://doi.org/10.1149/07208.0131ecst
 被引用回数：1 パーセンタイル：48.91(Electrochemistry)

The electronic structures of Pt and Pt-Co nanoparticles with O$$_{2}$$ adsorption and O$$_{2}$$/H$$_{2}$$O co-adsorption were investigated by in situ hard X-ray photoelectron spectroscopy (HAXPES) and in situ high resolution fluorescence detection X-ray absorption spectroscopy (HERFD-XAS) to clarify the effects of water adsorption on fuel cell cathode catalysis surface. The experimental results suggest that under the pressure of 1 mbar, the adsorption of H$$_{2}$$O hinders the successive O$$_{2}$$ adsorption on Pt surface, while under the pressure of 1 bar, the adsorption of H$$_{2}$$O enhances the adsorption of O$$_{2}$$ on Pt surface. This water effect is found to be more significant on Pt surface than on Pt-Co surface. These results would be helpful to understand how the water affects the fuel cell performance and why Pt-Co nanoparticles show higher oxygen reduce reaction (ORR) activity than Pt nanoparticles.

論文

Resonant inelastic X-ray scattering study of entangled spin-orbital excitations in superconducting PrFeAsO$$_{0.7}$$

野村 拓司*; 原田 慈久*; 丹羽 秀治*; 石井 賢司*; 石角 元志*; 社本 真一; Jarrige, I.*

Physical Review B, 94(3), p.035134_1 - 035134_9, 2016/07

https://doi.org/10.1103/PhysRevB.94.035134
 被引用回数：11 パーセンタイル：47.12(Materials Science, Multidisciplinary)

Fe-$$L_{3}$$吸収端での共鳴非弾性X線散乱(RIXS)を用いて、典型的な鉄系超伝導体PrFeAsO$$_{0.7}$$の単結晶で、低エネルギー電子励起スペクトルを測定した。

論文

Observation of momentum-resolved charge fluctuations proximate to the charge-order phase using resonant inelastic X-ray scattering

吉田 雅洋*; 石井 賢司; 中 惇*; 石原 純夫*; Jarrige, I.*; 池内 和彦*; 村上 洋一*; 工藤 一貴*; 小池 洋二*; 永田 知子*; et al.

Scientific Reports (Internet), 6, p.23611_1 - 23611_8, 2016/03

https://doi.org/10.1038/srep23611
 被引用回数：1 パーセンタイル：11.46(Multidisciplinary Sciences)

In strongly correlated electron systems, enhanced fluctuations in the proximity of the ordered states of electronic degrees of freedom often induce anomalous electronic properties such as unconventional superconductivity. While spin fluctuations in the energy-momentum space have been studied widely using inelastic neutron scattering, other degrees of freedom, i.e., charge and orbital, have hardly been explored thus far. Here, we use resonant inelastic X-ray scattering to observe charge fluctuations proximate to the charge-order phase in transition metal oxides. In the two-leg ladder of Sr$$_{14-x}$$Ca$$_x$$Cu$$_{24}$$O$$_{41}$$, charge fluctuations are enhanced at the propagation vector of the charge order ($$mathbf{q}_mathrm{CO}$$) when the order is melted by raising the temperature or by doping holes. In contrast, charge fluctuations are observed not only at $$mathbf{q}_mathrm{CO}$$ but also at other momenta in a geometrically frustrated triangular bilayer lattice of LuFe$$_2$$O$$_4$$. The observed charge fluctuations have a high energy ($$sim$$ 1 eV), suggesting that the Coulomb repulsion between electrons plays an important role in the formation of the charge order.

論文

共鳴非弾性X線散乱を用いた強相関電子系研究の進展

石井 賢司

固体物理, 51(2), p.79 - 92, 2016/02

In the last decade, resonant inelastic X-ray scattering for the study of electronic excitations in strongly correlated electron systems has achieved significant progress utilizing brilliant synchrotron radiation X-rays. Some representative studies on cuprates and iridates are reviewed.

論文

Large trigonal-field effect on spin-orbit coupled states in a pyrochlore iridate

植松 大介*; 佐賀山 基*; 有馬 孝尚*; 石川 洵*; 中辻 知*; 高木 英典*; 吉田 雅洋*; 水木 純一郎; 石井 賢司

Physical Review B, 92(9), p.094405_1 - 094405_6, 2015/09

https://doi.org/10.1103/PhysRevB.92.094405
 被引用回数：22 パーセンタイル：66.77(Materials Science, Multidisciplinary)

The half-filled topmost valence band of Ir$$^{4+}$$ in several iridates such as Sr$$_2$$IrO$$_4$$, IrO$$_2$$, and CaIrO$$_3$$ has been proposed to originate mainly from the spin-orbit coupled $$J_{rm eff}=1/2$$ states. In pyrochlore iridates $$R_2$$Ir$$_2$$O$$_7$$ ($$R$$: rare earth), some exotic electronic states are theoretically proposed by assuming $$J_{rm eff}=1/2$$ states. However, the octahedral coordination around Ir is trigonally distorted, which may affect the energy level scheme of Ir $$5d$$ states. Here, we report spectra of resonant elastic and inelastic X-ray scattering in Eu$$_2$$Ir$$_2$$O$$_7$$ at the Ir $$L$$ edges. A large suppression of the magnetic scattering signal at the Ir $$L_{rm II}$$ edge supports the $$J_{rm eff}=1/2$$ picture rather than the $$S=1/2$$ one. The inelastic scattering spectrum indicates that the magnitude of the trigonal field on the Ir$$^{4+}$$ states is evaluated to be comparable to the spin-orbit interaction. The energy diagram of the $$5d$$ state is proposed based on the simple cluster model.

論文

Engineering a spin-orbital magnetic insulator by tailoring superlattices

松野 丈夫*; 井原 康太*; 山村 周玄*; 和達 大樹*; 石井 賢司; Shankar, V.*; Kee, H.-Y.*; 高木 英典*

Physical Review Letters, 114(24), p.247209_1 - 247209_5, 2015/06

https://doi.org/10.1103/PhysRevLett.114.247209
 被引用回数：148 パーセンタイル：97.75(Physics, Multidisciplinary)

In $$5d$$ Ir oxides with interplay of spin-orbit coupling and electron correlations, we have tailored a spin-orbital magnetic insulator out of a semimetal SrIrO$$_3$$ by tuning the structure through superlattices [(SrIrO$$_3$$)$$_m$$, SrTiO$$_3$$] ($$m$$ = 1, 2, 3, 4, and $$infty$$). We observed the systematic decrease of the magnetic ordering temperature and the resistivity as a function of $$m$$. The transition from the semimetal to the insulator is found to be closely linked to the appearance of magnetism at $$m$$ $$simeq$$ 3. Long range magnetic ordering was realized even in the $$m$$ = 1 single layer superlattice, implying that the design and realization of novel electronic phases is feasible at the level of a single atomic layer in complex Ir oxides.

論文

Extending resonant inelastic X-ray scattering to the extreme ultraviolet

Wray, L. A.*; Huang, S.-W.*; Jarrige, I.*; 池内 和彦*; 石井 賢司; Li, J.*; Qiu, Z. Q.*; Hussain, Z.*; Chuang, Y.-D.*

Frontiers in Physics (Internet), 3, p.32_1 - 32_11, 2015/05

https://doi.org/10.3389/fphy.2015.00032
 被引用回数：4

In resonant inelastic X-ray scattering (RIXS), core hole resonance modes are used to enhance coupling between photons and low energy electronic degrees of freedom. Resonating with shallow core holes accessed in the extreme ultraviolet (EUV) can provide greatly improved energy resolution at standard resolving power, but has been found to often yield qualitatively different spectra than similar measurements performed with higher energy X-rays. This paper uses experimental data and multiplet-based numerical simulations for the M-edges of Co-, Ni-, and Cu-based Mott insulators to review the properties that distinguish EUV RIXS from more commonly performed higher energy measurements. Key factors such as the origin of the strong EUV elastic line and advantages of EUV spectral functions over soft X-ray RIXS for identifying intrinsic excitation line shapes are discussed.

論文

High-energy magnetic excitations in overdoped La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ studied by neutron and resonant inelastic X-ray scattering

脇本 秀一; 石井 賢司; 木村 宏之*; 藤田 全基*; Dellea, G.*; Kummer, K.*; Braicovich, L.*; Ghiringhelli, G.*; Debeer-Schmitt, L. M.*; Granroth, G.*

Physical Review B, 91(18), p.184513_1 - 184513_7, 2015/05

https://doi.org/10.1103/PhysRevB.91.184513
 被引用回数：28 パーセンタイル：73.7(Materials Science, Multidisciplinary)

We have performed neutron inelastic scattering and resonant inelastic X-ray scattering (RIXS) at the Cu-$$L_3$$ edge to study high-energy magnetic excitations at energy transfers of more than 100 meV for overdoped La$$_{2-x}$$Sr$$_{x}$$CuO$$_{4}$$ with $$x$$ = 0.25 ($$T_c$$ = 15 K) and $$x$$ = 0.30 (nonsuperconducting) using identical single-crystal samples for the two techniques. Our results indicate consistency between neutron inelastic scattering and RIXS, and elucidate the entire magnetic excitation in the $$(pi, pi)$$ direction by the complementary use of two probes. The paramagnon along $$(pi, 0)$$ agrees well with the LCO spin-wave dispersion, while the paramagnon in the $$(pi, pi)$$ direction probed by RIXS appears to be less dispersive.

論文

Kondo interactions from band reconstruction in YbInCu$$_4$$

Jarrige, I.*; 小谷 章雄*; 山岡 人志*; 辻井 直人*; 石井 賢司; Upton, M.*; Casa, D.*; Kim, J. H.*; Gog, T.*; Hancock, J. N.*

Physical Review Letters, 114(12), p.126401_1 - 126401_5, 2015/03

https://doi.org/10.1103/PhysRevLett.114.126401
 被引用回数：11 パーセンタイル：60.87(Physics, Multidisciplinary)

We combine resonant inelastic X-ray scattering and model calculations in the Kondo lattice compound YbInCu$$_4$$, a system characterized by a dramatic increase in Kondo temperature and associated valence fluctuations below a first-order valence transition at T $$simeq$$ 42 K. The bulk-sensitive, element-specific, and valence-projected charge excitation spectra reveal an unusual quasigap in the Yb-derived state density which drives an instability of the electronic structure and renormalizes the low-energy effective Hamiltonian at the transition. Our results provide long-sought experimental evidence for a link between temperature-driven changes in the low-energy Kondo scale and the higher-energy electronic structure of this system.

論文

Towards optimizing the performance of self-regenerating Pt-based perovskite catalysts

Jarrige, I.*; 石井 賢司; 松村 大樹; 西畑 保雄; 吉田 雅洋*; 岸 浩史*; 谷口 昌司*; 上西 真里*; 田中 裕久*; 笠井 秀明*; et al.

ACS Catalysis, 5(2), p.1112 - 1118, 2015/02

https://doi.org/10.1021/cs501608k
 被引用回数：18 パーセンタイル：43.96(Chemistry, Physical)

Self-regenerating automotive catalysts owe their remarkable performance to the repeated motion of the precious metal atoms in and out of the perovskite lattice under fluctuating oxidizing and reducing conditions, preventing coalescence of the metal nanoparticles. Here we use resonant inelastic X-ray scattering to characterize the occupied and unoccupied Pt 5d states in two self-regenerating Pt-perovskite catalysts, CaTi$$_{0.95}$$Pt$$_{0.05}$$O$$_3$$ and CaZr$$_{0.95}$$Pt$$_{0.05}$$O$$_3$$. Upon reduction, the element and symmetry-specific charge excitation spectra reveal a sizeable hybridization between the Pt 5d and the Ti 3d or Zr 4d states at the interface between the nanoparticles and the perovskite, which involves the occupied states and is thus invisible in X-ray absorption spectra. A correlation is found between the strength of this d-band hybridization and the proportion of Pt nanoparticles that remain buried below the surface during reduction, indicating that the motion of the Pt atoms towards the surface is hindered by this hybridization specifically, rather than by the Pt-O bonding. These results provide direct evidence that the strength of the metal-metal d-band hybridization plays a pivotal role in determining the efficiency of self-regeneration in perovskite catalysts.

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