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Spectroscopic techniques, including photoelectron spectroscopy, diffuse reflectance, and x-ray absorption, are used to investigate the electronic structure and the local structure of LaOBiS$_{2-x}$Se$_x$ thermoelectric material. It is found that Se substitution effectively suppresses local distortion, that can be responsible for the increased carrier mobility together with a change in the electronic structure. The results suggest a possible way to control thermoelectric properties by tuning of the local crystal structure of these materials., Comment: 6 pages, 4 figures, 1 table, J. Appl. Phys. (in press)

Using high-resolution spin-resolved photoemission spectroscopy, we observed a thermal spin depolarization to which all spin-polarized electrons contribute. Furthermore we observed a distinct minority spin state near the Fermi level and a corresponding depolarization that seldom contributes to demagnetization. The origin of this depolarization has been identified as the many-body effect characteristics of half-metallic ferromagnets. Our investigation opens an experimental field of itinerant ferromagnetic physics focusing on phenomena with sub-meV energy scale., Comment: 19 pages, 10 figures

The local structures of 122-type paradium arsenides, namely BaPd$_2$As$_2$ and SrPd$_2$As$_2$, are examined by As K-edge extended x-ray absorption fine structure measurements to find a possible correlation between the variation of their superconducting transition temperature and the local structure. The local atomic distances are found to be consistent with average distances measured by diffraction techniques. The temperature dependence of mean square relative displacements reveal that, while BaPd$_2$As$_2$ is characterized by a local As-Pd soft mode, albeit with larger atomic disorder, SrPd$_2$As$_2$ shows anomalous As-Pd correlations with a kink at $\sim$160 K due to hardening by raising temperature. We have discussed implications of these results and possible mechanism of differing superconducting transition temperature in relation with the structural instability., Comment: Main text: 5 pages, 4 figures, Supplemental information: 2 pages, 1 figure, 1 table

The local structure of correlated spin-orbit insulator Sr$_{2-x}$M$_x$IrO$_4$ (M = K, La) has been investigated by Ir L$_3$-edge extended x-ray absorption fine structure measurements. The measurements were performed as a function of temperature for different dopings induced by substitution of Sr with La or K. It is found that Ir-O bonds have strong covalency and they hardly show any change across the N\'eel temperature. In the studied doping range, neither Ir-O bonds nor their dynamics, measured by their mean square relative displacements, show any appreciable change upon carrier doping, indicating possibility of a nanoscale phase separation in the doped system. On the other hand, there is a large increase of the static disorder in Ir-Sr correlation, larger for K doping than La doping. Similarities and differences with respect to the local lattice displacements in cuprates are briefly discussed., Comment: Main text: 6 pages, 4 figures, Supplemental information: 2 pages, 2 figures

Synchrotron-based angle-resolved photoemission spectroscopy is used to determine the electronic structure of layered SnSe, which was recently turned out to be a potential thermoelectric material. We observe that the top of the valence band consists of two nearly independent hole bands, whose tops differ by ~20 meV in energy, indicating the necessity of a multivalley model to describe the thermoelectric properties. The estimated effective masses are anisotropic, with in-plane values of 0.16-0.39 m$_0$ and an out-of-plane value of 0.71 m$_0$, where m$_0$ is the rest electron mass. Information of the electronic structure is essential to further enhance the thermoelectric performance of hole-doped SnSe., Comment: 14 pages including 2 figures + 2 pages of supplementary data

Electronic structure has been studied in lightly electron doped correlated spin-orbit insulator Sr$_2$IrO$_4$ by angle-resolved photoelectron spectroscopy. We have observed coexistence of the lower Hubbard band and the in-gap band, the momentum dependence of the latter traces that of the band calculations without on-site Coulomb repulsion. The in-gap state remained anisotropically gapped in all observed momentum area, forming a remnant Fermi surface state, evolving towards the Fermi energy by carrier doping. These experimental results show a striking similarity with those observed in deeply underdoped cuprates, suggesting the common nature of the nodal liquid states observed in both compounds., Comment: 6 pages, 5 figures + Supplemental Material(4 pages, 5 figures), accepted for publication in PRB

The electronic structure of nearly optimally-doped novel superconductor LaO$_{1-x}$F$_x$BiS$_2$ (${\it x}$ = 0.46) was investigated using angle-resolved photoemission spectroscopy (ARPES). We clearly observed band dispersions from 2 to 6 eV binding energy and near the Fermi level (${\it E}_{\rm F}$), which are well reproduced by first principles calculations when the spin-orbit coupling is taken into account. The ARPES intensity map near ${\it E}_{\rm F}$ shows a square-like distribution around the $\Gamma$(Z) point in addition to electronlike Fermi surface (FS) sheets around the X(R) point, indicating that FS of LaO$_{0.54}$F$_{0.46}$BiS$_2$ is in close proximity to the theoretically-predicted topological change., Comment: 6 pages, 3 figures, + supplemental material

We use photoemission spectroscopy to study electronic structures of pristine and K-doped solid picene. The valence band spectrum of pristine picene consists of three main features with no state at the Fermi level (EF), while that of K-doped picene has three structures similar to those of pristine picene with new states near EF, consistent with the semiconductor-metal transition. The K-induced change cannot be explained with a simple rigid-band model of pristine picene, but can be interpreted by molecular orbital calculations considering electron-intramolecular-vibration interaction. Excellent agreement of the K-doped spectrum with the calculations points to importance of electron-intramolecular-vibration interaction in K-doped picene., Comment: This article is accepted by Physical Review B

We report on the muon spin rotation/relaxation study of a pyrochlore oxide, Cd2Os2O7, which exhibits a metal-insulator (MI) transition at T_{MI}~225 K without structural phase transition. It reveals strong spin fluctuation (>10^8/s) below the MI transition, suggesting a predominant role of geometrical spin frustration amongst Os^{5+} ions. Meanwhile, upon further cooling, a static spin density wave discontinuously develops below T_{SDW}~150 K. These observations strongly suggest the occurrence of an anomalous magnetic transition and associated change in the local spin dynamics in undistorted pyrochlore antiferromagnet., Comment: 5 pages, 4 figures

We have measured photoemission spectra of two kinds of TiO$_2$-capped VO$_2$ thin films, namely, that with rutile-type TiO$_2$ (r-TiO$_2$/VO$_2$) and that with amorphous TiO$_2$ (a-TiO$_2$/VO$_2$) capping layers. Below the Metal-insulator transition temperature of the VO$_2$ thin films, $\sim 300$ K, metallic states were not observed for the interfaces with TiO$_2$, in contrast with the interfaces between the band insulator SrTiO$_3$ and the Mott insulator LaTiO$_3$ in spite of the fact that both TiO$_2$ and SrTiO$_3$ are band insulators with $d^0$ electronic configurations and both VO$_2$ and LaTiO$_3$ are Mott insulators with $d^1$ electronic configurations. We discuss possible origins of this difference and suggest the importance of the polarity discontinuity of the interfaces. Stronger incoherent part was observed in r-TiO$_2$/VO$_2$ than in a-TiO$_2$/VO$_2$, suggesting Ti-V atomic diffusion due to the higher deposition temperature for r-TiO$_2$/VO$_2$., Comment: 5 pages, 6 figures

We report nuclear magnetic resonance studies on the beta-pyrochlore oxide superconductor KOs2O6. The nuclear relaxation at the K sites is entirely caused by fluctuations of electric field gradient, which we ascribe to highly anharmonic low frequency oscillation (rattling) of K ions. A phenomenological analysis shows a crossover from overdamped to underdamped behavior of the rattling phonons with decreasing temperature and its sudden sharpening below the superconducting transition temperature Tc. Absence of the Hebel-Slichter peak in the relaxation rate at the O sites below Tc also indicates strong electron-phonon coupling., Comment: 4 pages, 3 figures

The temperature ($T$) dependent metal-insulator transition (MIT) in VO$_2$ is investigated using bulk sensitive hard x-ray ($\sim$ 8 keV) valence band, core level, and V 2$p-3d$ resonant photoemission spectroscopy (PES). The valence band and core level spectra are compared with full-multiplet cluster model calculations including a coherent screening channel. Across the MIT, V 3$d$ spectral weight transfer from the coherent ($d^1\underbar{\it {C}}$ final) states at Fermi level to the incoherent ($d^{0}+d^1\underbar{\it {L}}$ final) states, corresponding to the lower Hubbard band, lead to gap-formation. The spectral shape changes in V 1$s$ and V 2$p$ core levels as well as the valence band are nicely reproduced from a cluster model calculations, providing electronic structure parameters. Resonant-PES finds that the $d^1\underbar{\it{L}}$ states resonate across the V 2$p-3d$ threshold in addition to the $d^{0}$ and $d^1\underbar{\it {C}}$ states. The results support a Mott-Hubbard transition picture for the first order MIT in VO$_2$., Comment: 6 pages, 3 figures. to be published in Phys. Rev. B

We have investigated the charge dynamics of VO2 by optical reflectivity measurements. Optical conductivity clearly shows a metal-insulator transition. In the metallic phase, a broad Drude-like structure is observed. On the other hand, in the insulating phase, a broad peak structure around 1.3 eV is observed. It is found that this broad structure observed in the insulating phase shows a temperature dependence. We attribute this to the electron-phonon interaction as in the photoemission spectra., Comment: 6 pages, 8 figures, accepted for publication in Phys. Rev. B

To elucidate the nature of the superconducting ground state of the geometrically frustrated pyrochlore KOs2O6 (Tc=9.6K), the thermal conductivity was measured down to low temperatures (~Tc/100). We found that the quasiparticle mean free path is strikingly enhanced below a transition at Tp=7.5K, indicating enormous electron inelastic scattering in the normal state. In a magnetic field the conduction at T ->0K is nearly constant up to ~0.4Hc2, in contrast with the rapid growth expected for superconductors with an anisotropic gap. This unambiguously indicates a fully gapped superconductivity, in contrast to the previous studies. These results highlight that KOs2O6 is unique among superconductors with strong electron correlations., Comment: 5 pages, 4 figures, accepted for publication in Phys. Rev. Lett

A novel metallic and magnetic transition metal oxide Ag2NiO2 is studied by means of resistivity, magnetic susceptibility, specific heat and X-ray diffraction. The crystal structure is characterized by alternating stacking of a Ni3+O2 layer and a (Ag2)+ layer, the former realizing a spin-1/2 triangular lattice with eg orbital degeneracy and the latter providing itinerant electrons. It is found that the NiO2 layer exhibits orbital ordering at Ts = 260 K and antiferromagnetic spin ordering at TN = 56 K. Moreover, a moderately large mass enhancement is found for the itinerant electrons, suggesting a significant contribution from the nearly localized Ni 3d state to the Ag 5s state that forms a broad band., Comment: 9 pages, 5 figures, to be published in Rapid Communications, Phys. Rev. B

High pressure effects on the superconducting transitions of beta-pyrochlore superconductors AOs2O6 (A = Cs, Rb, K) are studied by measuring resistivity under high pressures up to 10 GPa. The superconducting transition temperature Tc first increases with increasing pressure in all the compounds and then exhibits a broad maximum at 7.6 K (6 GPa), 8.2 K (2 GPa) and 10 K (0.6 GPa) for A = Cs, Rb and K, respectviely. Finally, the superconductivity is suppressed completely at a critical pressure near 7 GPa and 6 GPa for A = Rb and K and probably above 10 GPa for A = Cs. Characteristic changes in the coefficinet A of the T2 term in resistivity and residual resistivity are observed, both of which are synchronized with the corresponding change in Tc. It is suggested that electron correlations and certain quantum fluctuations play important roles in the occurrence or suppression of superconductivity in the beta-pyrochlore oxides., Comment: 6 pages, 4 figures

This paper has been withdrawn by the authors, since a crucial assumption in the analysis of the data was found to be incorrect from the later experiments., Comment: This paper has been withdrawn

We report the discovery of a new pyrochlore oxide superconductor RbOs2O6. The compound crystallizes in the same beta-pyrochlore structure as the recently discovered superconductor KOs2O6, where Os atoms form a corner-sharing tetrahedral network called the pyrochlore lattice with Rb or K atoms in the cage. Resistivity, magnetic susceptibility and specific heat measurements on polycrystalline samples evidence a bulk superconductivity with Tc = 6.3 K.

Magnetic penetration depth ($\lambda$) in a pyrochlore superconductor KOs$_2$O$_6$ was studied by means of muon spin rotation (\msr). The temperature dependence of transverse spin relaxation rate, which is proportional to $\lambda ^{-2}$, exhibits a considerable deviation from that expected for the empirical two-fluid model ($\propto T^4$), rather obeying a $T^2$-tendency. Furthermore, $\lambda$ apparently increases with increasing applied field, suggesting the presence of nonlinear and nonlocal effects. These findings strongly suggest that the superconducting order parameter in KOs$_2$O$_6$ is anisotropic., Comment: 5 pages, 3 figures, submitted to J. Phys.: Cond. Matt

Superconductivity in the potassium osmium oxide KOs2O6 crystallizing in the beta-pyrochlore structure is studied by means of electrical resistivity, magnetic susceptibility and specific heat. It is the second superconductor in the family of pyrochlore oxides, following the alfa-type pyrochlore oxide Cd2Re2O7 which is believed to be a conventional s-wave superconductor. The superconducting transition temperature Tc of KOs2O6 is 9.6 K, almost one order higher than the Tc = 1.0 K of Cd2Re2O7. Moreover, the superconductivity of KOs2O6 is remarkably robust under high magnetic fields, with a large upper critical magnetic field Hc2 of about 38 T, which seems to exceed Pauli's limit expected for conventional superconductivity. This is also in contrast to the case of Cd2Re2O7, in which the Hc2 is 0.29 T, much smaller than the corresponding Pauli's limit. These distinct contrasts strongly suggest that the mechanism of superconductivity is essentially different between the two pyrochlore oxides., Comment: This paper has been withdrawn by the authors, due to a crucial error in the magnitude of magnetic fields used in the experiments

We have made a detailed temperature-dependent photoemission study of VO_2/TiO_2(001) thin films, which show a metal-insulator transition at \sim 300 K. Clean surfaces were obtained by annealing the films in an oxygen atmosphere. Spectral weight transfer between the coherent and incoherent parts accompanying the metal-insulator transition was clearly observed. We also observed a hysteretic behavior of the spectra for heating-cooling cycles. We have derived the ``bulk'' spectrum of the metallic phase and found that it has a strong incoherent part. The width of the coherent part is comparable to that given by band-structure calculation in spite of its reduced spectral weight, indicating that the momentum dependence of the self-energy is significant. This is attributed to by ferromagnetic fluctuation arising from Hund's rule coupling between different d orbitals as originally proposed by Zylbersztejn and Mott. In the insulating phase, the width of the V 3d band shows strong temperature dependence. We attribute this to electron-phonon interaction and have reproduced it using the independent boson model with a very large coupling constant., Comment: 7 pages, 7 figures, submitted to Phys. Rev. B

This paper has been withdrawn by the author(s), due a crucial error in the data.

Electronic properties of the metallic pyrochlore oxide Cd2Re2O7 are studied by means of electrical resistivity and Hall measurements. Semimetallic band structures are revealed as expected from band structure calculations. It is found that large changes in carrier density and mass occur at the structural phase transition at Ts1 = 200 K. A large mass enhancement is observed, particularly for the high-temperature phase with the ideal pyrochlore structure, suggesting that an anomalous correlation has an important effect on the itinerant electrons in the pyrochlore lattice., Comment: 4 pages, 4 figures, J. Phys. Soc. Jpn., in press

We report a structural phase transition found at Ts = 200 K in a pyrochlore oxide Cd2Re2O7 which shows superconductivity at Tc = 1.0 K. X-ray diffractionexperiments indicate that the phase transition is of the second order, from a high-temperature phase with the ideal cubic pyrochlore structure (space group Fd-3m) to a low-temperature phase with another cubic structure (space group F-43m). It is accompanied by a dramatic change in the resistivity and magnetic susceptibility and thus must induce a significant change in the electronic structure of Cd2Re2O7., Comment: 4 pages, 4figures, proceeding for ISSP8

We report the first pyrochlore oxide superconductor Cd2Re2O7. Resistivity,magnetic susceptibility,and specific heat measurements on single crystals evidence a bulk superconductivity at 1 K. Another phase transition found at 200 K suggests that a peculiar electronic structure lies behind the superconductivity., Comment: 4 pages, 4 figures, PRL, in press