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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:19.11(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

Electronic excitations around the substituted atom in La$$_2$$Cu$$_{1-y}$$N$$_y$$O$$_4$$ as seen via resonant inelastic X-ray scattering

石井 賢司; 筒井 健二; 池内 和彦*; Jarrige, I.; 水木 純一郎; 平賀 晴弘*; 山田 和芳*; 遠山 貴己*; 前川 禎通; 遠藤 康夫*; et al.

Physical Review B, 85(10), p.104509_1 - 104509_5, 2012/03

 被引用回数:3 パーセンタイル:14.95(Materials Science, Multidisciplinary)

We perform a resonant inelastic X-ray scattering (RIXS) study of Ni-substituted La$$_2$$CuO$$_4$$ and Cu-substituted La$$_2$$NiO$$_4$$.Resonantly enhanced charge-transfer excitations are successfully observed by tuning the incident photon energy to the $$K$$-edge of the substituted element. These excitations display a very weak momentum dependence, evidencing their local character. We find a shift in the energy of the onset edge of these features compared with the non-substituted compounds La$$_2$$CuO$$_4$$ and La$$_2$$NiO$$_4$$. This shift is quantitatively reproduced by exact diagonalization calculations of the RIXS spectra. RIXS is shown to be a powerful tool to probe the electronic states of substituted elements and to understand their interaction with surrounding atoms.

論文

Three dimensional atomic image of TlInSe$$_{2}$$ by X-ray fluorescence holography

三村 功次郎*; 細川 伸也*; 八方 直久*; Hu, W.; 林 好一*; 脇田 和樹*; 石井 啓文*; 吉村 政人*; Jeyakanthan, J.*; Mamedov, N.*

e-Journal of Surface Science and Nanotechnology (Internet), 9, p.273 - 276, 2011/07

Three dimensional (3D) atomic images around the Tl atoms in single crystal TlInSe$$_{2}$$ thermoelectric material in the incommensurate phase were reconstructed by using Tl LIII X-ray fluorescence holography measured at room temperature. Comparison of the experimentally obtained 3D images with the theoretically calculated ones suggests that only the Tl atoms have large spatial fluctuations, which are related to the incommensurate phase of this material.

論文

Three-dimensional atomic images of TlInSe$$_{2}$$ thermoelectric material obtained by X-ray fluorescence holography

細川 伸也*; 八方 直久*; 林 好一*; 三村 功次郎*; 脇田 和樹*; Hu, W.; 石井 啓文*; 吉村 政人*; Jeyakanthan, J.*; Mamedov, N.*

Japanese Journal of Applied Physics, 50(5), p.05FC06_1 - 05FC06_2, 2011/05

 被引用回数:7 パーセンタイル:31.34(Physics, Applied)

Three dimensional (3D) atomic images around the Tl atoms in single crystal TlInSe$$_{2}$$ thermoelectric material in the incommensurate phase were reconstructed by using Tl $$L$$$$_{rm III}$$ X-ray fluorescence holography measured at room temperature. In the obtained 3D image, the In atoms are clearly visible at the proper positions in the normal phase. However, the Tl atomic images are also observed but very weak. By comparing the experimental image with a theoretically calculated one, it is concluded that only the Tl atoms have large spatial fluctuations, which are related to the incommensurate phase of this material.

論文

Resonant inelastic X-ray scattering of La$$_2$$Cu$$_{0.95}$$Ni$$_{0.05}$$O$$_4$$

石井 賢司; 池内 和彦*; Jarrige, I.; 水木 純一郎; 平賀 晴弘*; 山田 和芳*; 筒井 健二; 遠山 貴己*; 前川 禎通*; 遠藤 康夫*; et al.

Physica C, 470(Suppl.1), p.S155 - S157, 2010/12

 被引用回数:0 パーセンタイル:0(Physics, Applied)

Substitution of a specific element for a component is often used to elucidate its role in the superconductors. For a complete understanding of the substitution effect not only on the superconductivity but also on the electronic states, element-selective experiments are required. In this respect, resonant inelastic X-ray scattering (RIXS) has proven to be a powerful experimental technique enabling element-selective diagnosis of charge excitations. By tuning the incident photon energy to a given absorption edge of the element, the excitations involving the element are resonantly enhanced. In addition, RIXS has the advantage that momentum dependence can be measured. Using RIXS, we have measured the electronic excitations at the substituting sites in La$$_2$$Cu$$_{0.95}$$Ni$$_{0.05}$$O$$_4$$ and La$$_2$$Ni$$_{0.95}$$Cu$$_{0.05}$$O$$_4$$. Near the absorption edge of the substituting element, namely the Ni $$K$$-edge for La$$_2$$Cu$$_{0.95}$$Ni$$_{0.05}$$O$$_4$$ and the Cu $$K$$-edge for La$$_2$$Ni$$_{0.95}$$Cu$$_{0.05}$$O$$_4$$, charge transfer excitations from the 2$$p$$ level of neighboring oxygen to the upper Hubbard band of the substituted Ni/Cu are observed. Experimental spectra are qualitatively reproduced by a theoretical calculation based on a $$d$$-$$p$$ model.

論文

Thermally activated charge transfer in a Prussian blue derivative probed by resonant inelastic X-ray scattering

Jarrige, I.; Cai, Y. Q.*; 石井 啓文*; 平岡 望*; Bleuzen, A.*

Applied Physics Letters, 93(5), p.054101_1 - 054101_3, 2008/08

 被引用回数:9 パーセンタイル:36.51(Physics, Applied)

Charge-transfer excitation is at the source of the photoinduced magnetism observed in several Prussian blue molecule-based magnets. Using resonant inelastic X-ray scattering and X-ray absorption spectroscopy, we probe directly the thermally-activated charge transfer in a photomagnetic Fe-Co cyanide, Cs$$_{0.7}$$Co$$_{4}$$[Fe(CN)$$_{6}$$]$$_{2.9}$$[V]$$_{1.1}$$. 16H$$_{2}$$O, where [V] represents [Fe(CN)$$_{6}$$] vacancies. The temperature dependence of both Co and Fe valence ratios is estimated for the first time in one cooling run, thus yielding a more complete picture of the temperature-induced cooperative electronic modifications. This novel approach, benefiting from relatively short acquisition times, opens the possibility for realtime characterization of the photoinduced magnetism in molecule-based magnets.

口頭

Volume collapse transition in TmTe; Competition between strong correlation and $$f$$-$$d$$ hybridization at high pressure

Jarrige, I.; Rueff, J.-P.*; Shieh, S.*; 田口 宗孝*; 大石 泰生*; 松村 隆*; 石井 啓文*; 平岡 望*; Cai, Y.*

no journal, , 

The pressure-induced mixed-valent state in TmTe is investigated up to 10.6 GPa using resonant inelastic X-ray scattering (RIXS) and the Anderson impurity model (AIM). The volume collapse transition (VCT) which takes place over the 2-4.3 GPa range is accompanied by a strong increase in the 4$$f$$-5$$d$$ hybridization. The valence in the collapsed state is found to be 2.5, showing that the VCT is inconsistent with the commonly accepted picture of Tm$$^{2+}$$ to Tm$$^{3+}$$ conversion. At 6 GPa, a transition in both magnetic and electronic ground states occurs at constant valence and hybridization. This could be indicative of a non-trivial instability of the 4$$f$$ ground state such as a non Fermi liquid behavior.

口頭

Volume collapse transition in TmTe; Competition between strong correlation and f-d hybridization at high pressure

Jarrige, I.; Rueff, J.-P.*; Shieh, S.*; Wang, J.*; 松村 隆*; 石井 啓文*; 平岡 望*; Cai, Y.*

no journal, , 

The pressure-induced mixed-valent state in TmTe is investigated up to 10.6 GPa using resonant inelastic X-ray scattering (RIXS) and the Anderson impurity model (AIM). The volume collapse transition (VCT) which takes place over the 2$$sim$$4.3 GPa range is accompanied by a strong increase in the 4f-5d hybridization. The valence in the collapsed state is found to be $$sim$$2.5, showing that the VCT is inconsistent with the commonly accepted picture of Tm$$^{2+}$$ to Tm$$^{3+}$$ conversion. At 6 GPa, a transition in both magnetic and electronic ground states occurs at constant valence and hybridization. This could be indicative of a non-trivial instability of the 4f ground state such as a non Fermi liquid behavior.

口頭

LaMnO$$_{3}$$における圧力下金属絶縁体転移のX線発光と吸収分光法の測定

Jarrige, I.; Shieh, S.*; 石井 啓文*; 平岡 望*; Cai, Y.*

no journal, , 

Here we report on a spectroscopic investigation of the intricate interplays between electronic, magnetic and structural properties of LaMnO$$_{3}$$ across its pressure-induced insulator to metal transition (IMT) at 32 GPa. We measure the Mn K-beta fluorescence line by X-ray emission spectroscopy (XES) and the Mn K-egde by X-ray absorption spectroscopy in the partial fluorescence yield mode (PFY-XAS). The XES spectra disclose a high-spin to low-spin transition accompanying the IMT that points to strongly interwoven charge and spin degrees of freedom, which is reminiscent of the Mott perspective. On the other hand, close insight is gained on the structure from the Mn K pre-edge region, where evidence is found for a complete suppression of the Jahn-Teller distortions at the IMT. This is congruent with the scenario that the gap closure results from the progressive pressure-induced degeneracy of the majority-spin eg band, thus suggesting that the IMT in LaMnO$$_{3}$$ is not a plain Mott transition.

口頭

Ni置換La$$_2$$CuO$$_4$$の共鳴非弾性X線散乱

石井 賢司; 池内 和彦; Jarrige, I.; 水木 純一郎; 平賀 晴弘*; 山田 和芳*; 筒井 健二; 遠山 貴己*; 前川 禎通*; 石井 啓文*; et al.

no journal, , 

これまでに高温超伝導体のCuをNiに置換した系は非常に数多くの研究がなされてきた。その多くはCu$$^{2+}$$($$S=1/2$$)をNi$$^{2+}$$($$S=1$$)に置換したと考え、Niを磁性不純物として着目したものであったが、Ni置換は電子状態にも何らかの影響があると予想される。今回、共鳴非弾性X線散乱(RIXS)の元素選択性を利用することによりNi周りの電子状態を抽出することに成功したのでその結果について報告する。本研究で用いた$$K$$吸収端のRIXSでは、CuまたはNiの$$1s$$-$$4p$$遷移に対応するエネルギーのX線を利用することで、電荷ギャップを越える励起が観測できる。例えば、Niの$$K$$吸収端でLa$$_2$$Cu$$_{0.95}$$Ni$$_{0.05}$$O$$_4$$の測定を行うと、中間状態で生成されたNiの$$1s$$正孔を遮蔽するために周りの酸素$$2p$$軌道からNiの$$3d$$軌道へ電子が遷移する。酸素$$2p$$軌道にできたホールはCuとZhang-Rice siglet(ZRS)を形成するので、ZRSとNi($$3d^9$$)が存在するような励起状態を観測することになる。同様に、La$$_2$$CuO$$_4$$をCuの$$K$$吸収端で測定すると、ZRSとCu($$3d^{10}$$)が生じる励起状態が観測される。今回、La$$_2$$Cu$$_{1-y}$$Ni$$_y$$O$$_4$$$$y=0.05,0.95$$の測定を行い、既に報告されている$$y=0,1$$のスペクトルと比較することで、Ni, Cuそれぞれに特徴的な電子状態の議論を行う。

口頭

Competition between multi-channel Kondo effect and f delocalization in TmTe at high pressure

Jarrige, I.; Rueff, J.-P.*; Shieh, S.*; 田口 宗孝*; 石井 啓文*; Cai, Y. Q.*

no journal, , 

Identifying the mechanism of Kondo phenomena is arguably one of the most exciting and widely studied issues in condensed matter physics. Intermediate-valent Tm compounds stand out as potential candidates for multichannel Kondo (ncK) effect, since both integer valences Tm$$^{2+}$$ and Tm$$^{3+}$$ are magnetic. Using resonant inelastic X-ray scattering and the Anderson impurity model, we probed the Tm valence and 4f-5d hybridization in the high-pressure intermediate-valent TmTe compound. Our results reveal that the f delocalization is discontinuous, characterized by a previously unobserved plateau-like behavior over the 4.3$$sim$$6.5 GPa range. This is at odds with the usual, continuous Kondo-like f delocalization, and is interpreted as an experimental observation of the effect of culminating ncK scattering of d electrons from local moments on the electronic structure.

口頭

Competition between multi-channel Kondo effect and f delocalization in TmTe at high pressure

Jarrige, I.; Rueff, J.-P.*; Cai, Y. Q.*; Shieh, S.*; 石井 啓文*; 田口 宗孝*

no journal, , 

Among numerous f electron systems which present Kondo properties, intermediate-valent Tm compounds stand out as potential candidates for multichannel Kondo (ncK) effect, since both integer valences Tm2+ and Tm3+ are magnetic. Using resonant inelastic X-ray scattering and the Anderson impurity model, we probed the Tm valence and 4f-5d hybridization in the high-pressure intermediate-valent TmTe compound. Our results reveal that the f delocalization is discontinuous, characterized by a previously unobserved plateau-like behavior between the volume collapse transition and the structural transition (4.3$$sim$$6.5 GPa), with an associated valence (2.55) at odds with the near-trivalency previously reported. This is at odds with the usual, continuous Kondo-like f delocalization, and is interpreted as an experimental observation of the effect of culminating ncK scattering of d electrons from local moments on the electronic structure.

口頭

二次元検出器を用いた共鳴非弾性X線散乱の高分解能・高効率化

石井 賢司; Jarrige, I.; 池内 和彦; 吉田 雅洋; 石井 啓文*; 平岡 望*; 豊川 秀訓*

no journal, , 

近年、高輝度放射光を用いた共鳴非弾性X線散乱による電子励起状態の研究が行われるようになってきた。この手法を用いて物性とのかかわりの深い低エネルギーの励起を観測するためには、分光器の高分解能化は欠かせない。一方で、分解能を上げて検出するバンド幅を狭くすると検出効率が低下し、測定に時間がかかることになる。この点を克服するために、位置敏感型検出器を用いて複数のエネルギーを同時に測定する方法がHuotariらによって提案された。この方法は、最近APSの30IDに設置された分光器MERIXにおいても採用されている。この方法をSPring-8の非弾性ビームラインでも構築すべく、台湾ビームラインBL12XUでテスト実験を行った。検出器には、二次元ピクセルアレイ型のPILATUSを用いた。原理的には一次元検出器で可能であるが、二次元検出器を用いることで複数のアナライザーからの同時計測が可能になるなど、将来の拡張性が高い。結果、MnのK吸収端で約110meV、CuのK吸収端で約200meVの分解能を得た。講演では、現状の問題点,今後の展開と合わせて議論を行う予定である。

口頭

Single-channel vs multi-channel Kondo effects; SmTe and TmTe studied via resonant inelastic X-ray scattering under high pressure

Jarrige, I.; Rueff, J.-P.*; Shieh, S.*; 田口 宗孝*; 大石 泰生*; 松村 武*; 石井 啓文*; 平岡 望*; Cai, Y. Q.*

no journal, , 

Using resonant inelastic X-ray scattering and the Anderson impurity model, we estimated the pressure dependence of the Sm and Tm valence and 4 f -5d hybridization in the respectively single and multi-channel Kondo compounds SmTe and TmTe. We observed a usual, continuous Kondo-like f delocalization for SmTe as a function of pressure. On the contrary, our results reveal that the f delocalization in TmTe is discontinuous, characterized by a previously unobserved plateau-like behavior between 4.3 and 6.5 GPa. This is interpreted as an experimental observation of the effect of culminating multi-channel Kondo scattering of d electrons from local moments on the electronic structure. Our study raises the interesting possibility that an NCK effect realized in a compressed mixed-valent f system could impede the concomitant electron delocalization.

口頭

Electronic excitations probed with resonant inelastic X-ray scattering

石井 賢司; 筒井 健二; 池内 和彦*; Jarrige, I.; 水木 純一郎; 平賀 晴弘*; 山田 和芳*; 遠山 貴己*; 前川 禎通; 石井 啓文*; et al.

no journal, , 

It is widely recognized that inelastic scattering of neutron and X-ray is a powerful tool to investigate dynamical properties of electrons in the energy-momentum space. Especially, inelastic X-ray scattering has become available in the last decade by utilizing brilliant synchrotron radiation X-rays. When the incident X-ray energy is tuned to an absorption edge of a constituent element of materials, resonantly enhanced electronic excitations are observed, which is called resonant inelastic X-ray scattering (RIXS). An additional characteristic arises from the resonant process, namely, the specific element selectively get involved in the observed excitations. While neutron scattering is predominantly sensitive to spin excitations, one can complementarily measure various excitations of electronic degrees of freedom, charge, spin, and orbital, with the RIXS technique. In our presentation, we show an explicit application of the element selectivity: resonant inelastic X-ray scattering of Ni-substituted La$$_{2}$$CuO$$_{4}$$ and Cu-substituted La$$_{2}$$NiO$$_{4}$$. Resonantly enhanced charge-transfer excitations are successfully observed by tuning the incident photon energy to the K-edge of the substituted element. Combined with theoretical calculations, we will discuss the local electronic states around the substituted element which are affected through the interaction with surrounding atoms.

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