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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

 被引用回数:1 パーセンタイル:10.54(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

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

 被引用回数:25 パーセンタイル:67.70(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

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

 被引用回数:23 パーセンタイル:46.16(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.

論文

Spin-orbit coupling induced semi-metallic state in the 1/3 hole-doped hyper-kagome Na$$_3$$Ir$$_3$$O$$_8$$

高山 知弘*; Yaresko, A.*; 松本 章代*; Nuss, J.*; 石井 賢司; 吉田 雅洋*; 水木 純一郎; 高木 英典*

Scientific Reports (Internet), 4, p.6818_1 - 6818_6, 2014/10

 被引用回数:35 パーセンタイル:82.17(Multidisciplinary Sciences)

The complex iridium oxide Na$$_3$$Ir$$_3$$O$$_8$$ with a B-site ordered spinel structure was synthesized in single crystalline form, where the chiral hyper-kagome lattice of Irions, as observed in the spin-liquid candidate Na$$_4$$Ir$$_3$$O$$_8$$, was identified. The average valence of Ir is 4.33+ and, therefore, Na$$_3$$Ir$$_3$$O$$_8$$ can be viewed as a doped analogue of the hyper-kagome spin liquid with Ir$$^{4+}$$. The transport measurements, combined with the electronic structure calculations, indicate that the ground state of Na$$_3$$Ir$$_3$$O$$_8$$ is a low carrier density semi-metal. We argue that the semi-metallic state is produced by a competition of the molecular orbital splitting of $$t_{2g}$$ orbitals on Ir$$_3$$ triangles with strong spin-orbit coupling inherent to heavy Ir ions.

論文

High-energy spin and charge excitations in electron-doped copper oxide superconductors

石井 賢司; 藤田 全基*; 佐々木 隆了*; Minola, M.*; Dellea, G.*; Mazzoli, C.*; Kummer, K.*; Ghiringhelli, G.*; Braicovich, L.*; 遠山 貴己*; et al.

Nature Communications (Internet), 5, p.3714_1 - 3714_8, 2014/04

 被引用回数:98 パーセンタイル:94.33(Multidisciplinary Sciences)

We combine X-ray and neutron inelastic scattering measurements to track the doping dependence of both spin and charge excitations in electron-doped materials. Copper $$L_3$$ resonant inelastic X-ray scattering spectra show that magnetic excitations shift to higher energy upon doping. Their dispersion becomes steeper near the magnetic zone center and they deeply mix with charge excitations, indicating that electrons acquire a highly itinerant character in the doped metallic state. Moreover, above the magnetic excitations, an additional dispersing feature is observed near the $$Gamma$$-point, and we ascribe it to particle-hole charge excitations. These properties are in stark contrast with the more localized spin-excitations (paramagnons) recently observed in hole-doped compounds even at high doping-levels.

論文

Bipartite magnetic parent phases in the iron oxypnictide superconductor

平石 雅俊*; 飯村 壮史*; 小嶋 健児*; 山浦 淳一*; 平賀 晴弘*; 池田 一貴*; Miao, P.*; 石川 喜久*; 鳥居 周輝*; 宮崎 正範*; et al.

Nature Physics, 10(4), p.300 - 303, 2014/04

 被引用回数:108 パーセンタイル:95.02(Physics, Multidisciplinary)

High-temperature (high-$$T_{rm c}$$) superconductivity appears as a consequence of the carrier-doping of an undoped parent compound exhibiting antiferromagnetic order; thereby, ground-state properties of the parent compound are closely relevant to the superconducting state. On the basis of the concept, a spin-fluctuation has been addressed as an origin of pairing of the superconducting electrons in cuprates. Whereas, there is growing interest in the pairing mechanism such as an unconventional spin-fluctuation or an advanced orbital-fluctuation due to the characteristic multi-orbital system in iron-pnictides. Here, we report the discovery of an antiferromagnetic order as well as a unique structural transition in electron-overdoped LaFeAsO$$_{1-x}$$H$$_x$$ ($$x sim 0.5$$), whereby another parent phase was uncovered, albeit heavily doped. The unprecedented two-dome superconducting phases observed in this material can be interpreted as a consequence of the carrier-doping starting from the original at $$x sim 0$$ and advanced at $$x sim 0.5$$ parent phases toward the intermediate region. The bipartite parent phases with distinct physical properties in the second magnetic phase provide us with an interesting example to illustrate the intimate interplay among the magnetic interaction, structural change and orbital degree of freedom in iron-pnictides.

論文

Momentum-resolved resonant inelastic X-ray scattering on a single crystal under high pressure

吉田 雅洋*; 石井 賢司; Jarrige, I.*; 綿貫 徹; 工藤 一貴*; 小池 洋二*; 熊谷 健一*; 平岡 望*; 石井 啓文*; Tsuei, K.-D.*; et al.

Journal of Synchrotron Radiation, 21(1), p.131 - 135, 2014/01

 被引用回数:3 パーセンタイル:17.97(Instruments & Instrumentation)

A single-crystal momentum-resolved resonant inelastic X-ray scattering (RIXS) experiment under high pressure using an originally designed diamond anvil cell (DAC) is reported. The diamond-in/diamond-out geometry was adopted with both the incident and scattered beams passing through a 1 mm-thick diamond. This enabled us to cover wide momentum space keeping the scattering angle condition near 90$$^{circ}$$. Elastic and inelastic scattering from the diamond was drastically reduced using a pinhole placed after the DAC. Measurement of the momentum-resolved RIXS spectra of Sr$$_{2.5}$$Ca$$_{11.5}$$Cu$$_{24}$$O$$_{41}$$ at the Cu $$K$$-edge was thus successful. Though the inelastic intensity becomes weaker by two orders than the ambient pressure, RIXS spectra both at the center and the edge of the Brillouin zone were obtained at 3 GPa and low-energy electronic excitations of the cuprate were found to change with pressure.

論文

Instrumental upgrades of the RIXS spectrometer at BL11XU at SPring-8

石井 賢司; Jarrige, I.*; 吉田 雅洋*; 池内 和彦*; 稲見 俊哉; 村上 洋一*; 水木 純一郎

Journal of Electron Spectroscopy and Related Phenomena, 188, p.127 - 132, 2013/06

 被引用回数:13 パーセンタイル:57.03(Spectroscopy)

Two recent instrumental upgrades of the inelastic X-ray scattering spectrometer installed at BL11XU at SPring-8 are reported. The first one is a multianalyzer system, where we can simultaneously use three crystal analyzers aligned perpendicularly to the scattering plane. In a test measurement of polycrystalline $$alpha$$-PtO$$_2$$, the inelastic spectra obtained with each respective analyzer showed a completely identical lineshape, and a slight difference ($$le$$ 10%) in intensity. The system enhances the experimental efficiency, and allows for simultaneous scan at three momenta for a single-crystal sample. The second development is a polarization analyzer for the scattered photons. A pyrolytic graphite (PG) crystal is placed in front of the detector and serves as a polarization-analyzer crystal, using the (006) reflection for the Cu $$K$$-edge. We succeeded to observe clear polarization dependence in the $$d$$-$$d$$ excitations of KCuF$$_3$$.

論文

Resonant inelastic X-ray scattering study of intraband charge excitations in hole-doped high-$$T_c$$ cuprates

脇本 秀一; 石井 賢司; 木村 宏之*; 池内 和彦*; 吉田 雅洋*; 足立 匡*; Casa, D.*; 藤田 全基*; 福永 靖*; Gog, T.*; et al.

Physical Review B, 87(10), p.104511_1 - 104511_7, 2013/03

 被引用回数:10 パーセンタイル:41.31(Materials Science, Multidisciplinary)

We have performed resonant inelastic X-ray scattering (RIXS) near the Cu-$$K$$ edge on various cuprate superconductors, covering underdoped to heavily overdoped regimes and focusing on charge excitations inside the charge-transfer gap. RIXS measurements with $$E_i$$= 9.003 keV on metallic La$$_{1.7}$$Sr$$_{0.3}$$CuO$$_{4}$$ and Bi$$_{1.76}$$Pb$$_{0.35}$$Sr$$_{1.89}$$CuO$$_{6+delta}$$ exhibit a dispersive intraband excitation below 4 eV, similar to that observed in the electron-doped Nd$$_{1.85}$$Ce$$_{0.15}$$CuO$$_{4}$$. This is the first observation of a dispersive intraband excitation in a hole-doped system, evidencing that both electron- and hole-doped systems have a similar dynamical charge correlation function.

論文

Resonant inelastic X-ray scattering study of charge excitations in superconducting and nonsuperconducting PrFeAsO$$_{1-y}$$

Jarrige, I.*; 野村 拓司; 石井 賢司; Gretarsson, H.*; Kim, Y.-J.*; Kim, J.*; Upton, M.*; Casa, D.*; Gog, T.*; 石角 元志*; et al.

Physical Review B, 86(11), p.115104_1 - 115104_4, 2012/09

 被引用回数:8 パーセンタイル:33.79(Materials Science, Multidisciplinary)

鉄系高温超伝導体PrFeAsO$$_{0.7}$$とその親物質であるPrFeAsOに対して、運動量分解した共鳴非弾性X線散乱を初めて観測した。主な結果は次の2点である。まず、第一に、16バンドの$$dp$$模型を用いて、低エネルギーの励起が$$xz$$, $$yz$$軌道の特性を有する$$dd$$バンド内遷移に支配されていることを示し、電子相関に強く依存していることを示す。これによって、クーロン斥力$$U$$とフント結合$$J$$を見積もることができる。特に軌道依存した電子相関における$$J$$の果たす役割が明らかとなる。第二に、短距離の反強磁性相関が$$Gamma$$点での励起の説明には不可欠であることから、超伝導状態においてもそれが存在することが示される。

論文

Polarization-analyzed resonant inelastic X-ray scattering of the orbital excitations in KCuF$$_3$$

石井 賢司; 石原 純夫*; 村上 洋一*; 池内 和彦*; 葛下 かおり*; 稲見 俊哉; 大和田 謙二; 吉田 雅洋; Jarrige, I.; 多々見 央*; et al.

Physical Review B, 83(24), p.241101_1 - 241101_4, 2011/06

 被引用回数:21 パーセンタイル:62.69(Materials Science, Multidisciplinary)

We report a Cu $$K$$-edge resonant inelastic X-ray scattering (RIXS) study of orbital excitations in KCuF$$_3$$. By performing the polarization analysis of the scattered photons, we disclose that the excitation between the $$e_g$$ orbitals and the excitations from $$t_{2g}$$ to $$e_g$$ exhibit distinct polarization dependence. The polarization dependence of the respective excitations is interpreted based on a phenomenological consideration of the symmetry of the RIXS process that yields a necessary condition for observing the excitations. In addition, we show that the orbital excitations are dispersionless within our experimental resolution.

論文

Momentum-resolved electronic excitations in the Mott insulator Sr$$_2$$IrO$$_4$$ studied by resonant inelastic X-ray scattering

石井 賢司; Jarrige, I.; 吉田 雅洋; 池内 和彦*; 水木 純一郎; 大橋 啓*; 高山 知弘*; 松野 丈夫*; 高木 英典*

Physical Review B, 83(11), p.115121_1 - 115121_5, 2011/03

 被引用回数:73 パーセンタイル:90.53(Materials Science, Multidisciplinary)

We report an Ir $$L_3$$-edge resonant inelastic X-ray scattering (RIXS) measurement of the low-lying electronic excitations in Sr$$_2$$IrO$$_4$$ over the complete Brillouin zone of the IrO$$_2$$ plane. A remarkably strong inelastic signal which exceeds the elastic scattering in intensity is observed. Peaks observed at 0.5, 3.2, and 6.0 eV are respectively ascribed to an interband transition across the Mott gap and charge-transfer excitations from the O $$2p$$ band to the Ir $$5d$$ bands. The dispersion of the Mott gap excitation is found to be particularly weak. This is interpreted as a signature of the narrow $$5d$$ bands of the novel Mott insulating state of Sr$$_2$$IrO$$_4$$ induced by the strong spin-orbit interaction.

論文

Temperature dependence of the electronic structure of Sr$$_{14}$$Cu$$_{24}$$O$$_{41}$$ studied by resonant inelastic X-ray scattering

吉田 雅洋; 石井 賢司; 池内 和彦*; Jarrige, I.; 村上 洋一*; 水木 純一郎; 筒井 健二; 遠山 貴己*; 前川 禎通*; 工藤 一貴*; et al.

Physica C, 470(Suppl.1), p.S145 - S146, 2010/12

 被引用回数:4 パーセンタイル:20.84(Physics, Applied)

Sr$$_{14-x}$$Ca$$_x$$Cu$$_{24}$$O$$_{41}$$ (SCCO), which is composed of two-leg ladders and edge-sharing chains, is the first superconducting cuprate without CuO$$_2$$ planes. By substituting Ca for Sr, holes are transferred from the chains to the ladders. It was recently shown that charge ordering (CO) along the leg direction in the ladder occurs at $$x=0$$ and the periodicity is five times the unit length along the c axis. In order to investigate the electronic excitations associated with the CO, we carried out resonant inelastic X-ray scattering (RIXS) experiments for SCCO ($$x=0,6$$). Cu-$$K$$ RIXS can directly probe the momentum-dependent electronic excitations related to the Cu site, which are resonantly enhanced by tuning the incident photon energy to the Cu $$K$$-edge. We measured the q dependence of the intraband excitations, which is associated with the dynamics of doped holes in the Zhang-Rice singlet band. The intensity is enhanced at the momentum $${bf q}=(q_{rm rung},q_{rm leg})=(0,2pi/5)$$ corresponding to the periodicity of the CO in $$x=0$$, while the temperature dependence of the enhancement is different for $$x=0$$ and $$x=6$$. We discuss the relationship between our experimental results and the occurrence of the CO.

論文

Resonant inelastic X-ray scattering in single-crystal superconducting PrFeAsO$$_{0.7}$$

Jarrige, I.; 石井 賢司; 吉田 雅洋; 福田 竜生; 池内 和彦*; 石角 元志*; 平岡 望*; Tsuei, K.-D.*; 鬼頭 聖*; 伊豫 彰*; et al.

Physica C, 470(Suppl.1), p.S377 - S378, 2010/10

 被引用回数:4 パーセンタイル:20.84(Physics, Applied)

Resonant inelastic X-ray scattering (RIXS) spectra at the Fe K-edge were measured for a single-crystal of the iron oxypnictide superconductor PrFeAsO$$_{0.7}$$ ($$T_{rm C}$$ = 42 K). They disclose a weak, broad feature centered around 4.5 eV energy loss, which is slightly resonantly enhanced when the incident energy is tuned to the vicinity of the $$4p$$ white line. We tentatively ascribe it to the charge-transfer excitation between As $$4p$$ and Fe $$3d$$.

論文

Measurement of the spin and magnetic moment of $$^{23}$$Al

小澤 顕*; 松多 健策*; 長友 傑*; 三原 基嗣*; 山田 一成*; 山口 貴之*; 大坪 隆*; 百田 佐多夫*; 泉川 卓司*; 炭竃 聡之*; et al.

Physical Review C, 74(2), p.021301_1 - 021301_4, 2006/08

 被引用回数:44 パーセンタイル:88.92(Physics, Nuclear)

理化学研究所のリングサイクロトロンで、陽子過剰核$$^{23}$$Alの${it g}$因子を初めて測定した。実験的に測定された${it g}$因子の絶対値は、1.557$$pm$$0.088と決められた。この原子核は、鏡像核$$^{23}$$Neのエネルギー準位から見ると、基底状態は1/2$$^{+}$$もしくは5/2$$^{+}$$と考えられる。決められた${it g}$因子と殻模型計算による${it g}$因子との比較から1/2$$^{+}$$は明らかに否定されるため、基底状態のスピンは5/2$$^{+}$$と与えられた。これまで、$$^{23}$$Alは陽子ハロー構造のため、1/2$$^{+}$$状態が基底状態になる可能性が議論されてきたが、この実験により少なくとも基底状態にハロー構造が存在しないことがはっきりした。また、$$^{23}$$Neの磁気モーメントの実験値から、$$^{23}$$Alの基底状態におけるアイソスカラー固有スピンの期待値が求められるが、その値は$$^9$$Cのように異常な値を示さず、正常であることがわかった。

口頭

Pt-L3 resonant inelastic X-ray scattering on catalytic materials

Jarrige, I.; 松村 大樹; 石井 賢司; 吉田 雅洋; 水木 純一郎; 西畑 保雄

no journal, , 

Platinum is the most active catalyst, and as such is widely employed in automotive catalytic converters. We here report on the first use of RIXS at the Pt-L3 edge on catalytic and reference materials. RIXS spectra were measured on a foil of Pt metal, PtO$$_{2}$$ powder, and Pt and PtO$$_{2}$$ nanoparticles impregnated on Al$$_{2}$$O$$_{3}$$ powder, as a function of the incident energy across the Pt-L3 edge. The Raman features are all interpreted in terms of electron-hole excitations, dd excitations for Pt and dd excitations and charge transfer excitation from the occupied O 2p to the unoccupied Pt d states for PtO$$_{2}$$.

口頭

共鳴非弾性X線散乱によるSr$$_2$$IrO$$_4$$の電子励起

石井 賢司; Jarrige, I.; 吉田 雅洋; 池内 和彦*; 水木 純一郎; 大橋 啓*; 高山 知弘*; 松野 丈夫*; 高木 英典*

no journal, , 

近年、$$5d$$遷移金属を含んだ化合物において、強いスピン軌道相互作用に由来した特異な電子状態に注目が集まっている。その典型物質であるイリジウム酸化物Sr$$_2$$IrO$$_4$$は、スピン軌道相互作用と電子相関の効果によってギャップが開いたモット絶縁体であると考えられており、その電子状態をさまざまな分光法で検証することは重要である。われわれは、放射光X線を用いた電子励起の観測手法である共鳴非弾性X線散乱(Resonant Inelastic X-ray Scattering: RIXS)をこの系に適用し、Irの$$L_3$$吸収端での実験を行った。$$2p_{3/2}$$から$$5d$$軌道への遷移に対応する$$L_3$$吸収端の波長は約1${AA}$であり、励起の運動量依存性が観測可能である。まずは、1eV程度の比較的低いエネルギー分解能で、モットギャップを越える励起の分散関係を調べることを目的とした測定を行った。$$5d$$遷移金属の$$L$$吸収端を利用したRIXSの研究は、これまでにPt触媒に関する一報があるのみであり、本研究には分光学的な進展としての意義もある。

口頭

共鳴非弾性X線散乱によるSr$$_{14-x}$$Ca$$_{x}$$Cu$$_{24}$$O$$_{41}$$の電荷秩序と電荷励起

吉田 雅洋; 石井 賢司; Jarrige, I.; 池内 和彦*; 村上 洋一*; 水木 純一郎; 筒井 健二; 遠山 貴己*; 前川 禎通*; 工藤 一貴*; et al.

no journal, , 

二本足梯子格子系銅酸化物Sr$$_{14-x}$$Ca$$_{x}$$Cu$$_{24}$$O$$_{41}$$は、x$$geq$$9において高圧下で超伝導を示す。この物質の常圧基底状態として、共鳴軟X線回折実験から、母物質(x=0)と超伝導を示す組成(x$$sim$$11)でそれぞれ5倍, 3倍周期の静的な電荷秩序が報告されている。一方、マイクロ波伝導度の測定からは、x$$<$$9での基底状態がCDW状態であることが報告されている。2つの実験手法間で結果が完全に一致はしておらず、またx=0とx$$sim$$11での静的な電荷秩序の性質が同じであるかという点もまだ明らかになっていない。共鳴非弾性X線散乱(Resonant Inelastic X-ray Scattering: RIXS)は、一般的に入射X線により内殻電子を共鳴励起させ、その励起状態が緩和する過程で放出するX線を分光する手法で、励起の運動量変化を含めて直接電子状態を観測することができる。最近、遷移金属のK吸収端を用いたRIXSからストライプ型電荷秩序に関連した電荷励起が、約1eV付近のバンド内励起(ドープされたホールのZhang-Riceバンド内でのダイナミクスに対応)で観測されたが、二本足梯子格子系でも同様に、電荷秩序と関連した電荷励起が観測できることが期待される。そこで本研究では、Sr$$_{14-x}$$Ca$$_{x}$$Cu$$_{24}$$O$$_{41}$$の常圧基底状態に新しい知見を得ることを目的として、RIXSによる電荷秩序と関連する電荷励起の観測を試みた。これまでにx=0, 6の組成に関する結果を示してきたが、本講演では新たに測定したx=3, 9, 11.5での結果を加えて報告する。

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共鳴非弾性X線散乱におけるKCuF$$_3$$の軌道励起の偏光依存性

石井 賢司; 石原 純夫*; 村上 洋一*; 池内 和彦*; 葛下 かおり*; 大和田 謙二; 稲見 俊哉; 吉田 雅洋; Jarrige, I.; 多々見 央*; et al.

no journal, , 

近年、高輝度放射光光源を利用した数keV領域での共鳴非弾性X線散乱(RIXS)による物質の電子励起の研究が行われるようになってきている。このエネルギー領域は3$$d$$遷移金属のK吸収端に対応しており、運動量分解能,元素選択性といった利点があることから、遷移金属酸化物などの強相関電子系物質の電子状態の理解に大きな貢献が期待できる。共鳴X線回折における偏光解析が秩序パラメーターの対称性を決定できるのと同様に、RIXSでの偏光依存性は励起の対称性と密接な関係があると考えられる。ひとたび励起の対称性と偏光依存性に関する選択則が確立すれば、モデルのパラメーター値によらずに励起の起源の議論が可能となる。最初の偏光依存性の研究対象としてKCuF$$_3$$$$dd$$励起を選び、銅のK吸収端でのRIXS実験を行った。KCuF$$_3$$$$dd$$励起には大きく分けて、$$t_{2g}$$軌道から$$e_g$$軌道に電子が遷移するものと、$$e_g$$軌道間で電子が遷移するものがある。測定の結果、この2つの$$dd$$励起の偏光依存性に顕著な違いが存在することを発見した。K吸収端でのRIXSでは、双極子遷移による吸収・発光にかかわる$$4p$$軌道の対称性がX線の偏光と直接関係しており、$$3d$$-$$4p$$軌道間のクーロン相互作用についての群論的考察を行ったところ、「$$3d$$-$$4p$$相互作用の対称性から$$dd$$励起が起こるための必要条件が得られる」ことがわかった。

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Electronic excitations by resonant inelastic X-ray scattering

石井 賢司; 吉田 雅洋; Jarrige, I.; 池内 和彦*; 村上 洋一*; 水木 純一郎; 石原 純夫*; 筒井 健二; 遠山 貴己*; 前川 禎通; et al.

no journal, , 

In strongly correlated electron systems, such as transition metal oxides, it is widely recognized that the role of three degrees of freedom of the electron, i.e., charge, spin, and orbital are key ingredients to understand the electronic properties of these compounds. Among the degrees of freedom, dynamics of the spin in momentum-energy (Q-$$omega$$) space is studied by inelastic neutron scattering. On the other hand, photon is sensitive to the charge and its anisotropy, orbital, and therefore inelastic X-ray scattering (IXS) is suitable for the measurement of their excitations. In this sense, IXS can be considered as a complementary technique of the inelastic neutron scattering. Recently, brilliant X-rays from modern synchrotron radiation sources have enabled us to observe electronic excitations with IXS. Especially, resonant inelastic X-ray scattering (RIXS), where the incident photon energy is tuned near an absorption edge of a constituent element, has an advantage of significant resonant enhancement of inelastic signals and RIXS has been used to measure electronic excitations in strongly correlated electron systems. We will present our Cu K-edge RIXS works of charge-ordered Sr$$_{14}$$Cu$$_{24}$$O$$_{41}$$ and orbital-ordered KCuF$$_{3}$$ focusing on the charge and orbital excitations.

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