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We present Ir $4f$ core-level hard-x-ray photoemission spectroscopy (HAXPES) experiments conducted across antiferromagnetic (AFM) ordering transition in Ruddlesden-Popper iridates Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$. The Ir $4f$ spectra exhibit distinct changes between the AFM and paramagnetic (PM) phases, with the spectral difference $I_\text{PM}-I_\text{AFM}$ showing a contrasting behavior in the two compounds. By employing computational simulations using the local-density approximation combined with the dynamical mean-field theory method, we elucidate that $I_\text{PM}-I_\text{AFM}$ primary reflects the Slater or Mott-Hubbard character of the AFM insulating state rather than material specific details. This sensitivity to fine low-energy electronic structure arises from the dependence of charge-transfer responses to the sudden creation of a localized core hole on both metal-insulator transitions and long-range AFM ordering. Our result broadens the applications of core-level HAXPES as a tool for characterization of electronic structure., Comment: Main: 7 pages, 3 figures ; SM: 4 pages, 4 figures

We report the ground-state symmetry of the Ce $4f$ states in the heavy fermion superconductor CeNi$_{2}$Ge$_{2}$, yielding anisotropic $cf$-hybridization between the Ce $4f$ states and conducting electrons. By analyzing linear dichroism in soft x-ray absorption and core-level hard x-ray photoemission spectra, the $4f$ symmetry is determined as $\Sigma$-type $\Gamma_{7}$, promoting predominant hybridization with the conducting electrons originating from the Ge site. The band structures probed by the soft x-ray angle-resolved photoemission indicates that the Ge $4p$ components contribute to the band renormalization through the anisotropic hybridization effects, suggesting that the control of the electronic structures of Ge orbital gives an impact to achieve the exotic phenomena in CeNi$_{2}$Ge$_{2}$.

In this study, we investigate the bulk electronic structure of Pb-substituted LaO$_{0.5}$F$_{0.5}$BiS$_2$ single crystals, using two types of hard-x-ray spectroscopy. High-energy-resolution fluorescence-detected x-ray absorption spectroscopy revealed a spectral change at low temperatures. Using density functional theory (DFT) simulations, we find that the temperature-induced change originates from a structural phase transition, similar to the pressure-induced transition in LaO$_{0.5}$F$_{0.5}$BiS$_2$. This finding suggests that the mechanism of bulk superconductivity induced by Pb substitution is the same as that under high pressure. Furthermore, a novel low-valence state with a mixture of divalent and trivalent Bi ions is discovered using hard x-ray photoemission spectroscopy with the aid of DFT calculations., Comment: 8 pages, 6 figures, 1 table

We have probed the crystalline electric-field ground states of pure $|J = 7/2, J_z = \pm 5/2\rangle$ as well as the anisotropic $c$-$f$ hybridization in both valence fluctuating systems $\alpha$- and $\beta$-YbAlB$_4$ by linear polarization dependence of angle-resolved core level photoemission spectroscopy. Interestingly, the small but distinct difference between \abyb was found in the polar angle dependence of linear dichroism, indicating the difference in the anisotropy of $c$-$f$ hybridization which may be essential to a heavy Fermi liquid state in $\alpha$-YbAlB$_4$ and a quantum critical state in $\beta$-YbAlB$_4$.

We report experimentally observed linear dichroism in angle-resolved core-level photoemission spectra of PrIr2Zn20 and PrB6 in cubic symmetry. The different anisotropic 4f charge distributions between the compounds due to the crystalline-electric-field splitting are responsible for the difference in the linear dichroism, which has been verified by spectral simulations with the full multiplet theory for a single-site Pr3+ ion in cubic symmetry. The observed linear dichroism and polarization-dependent spectra in two different photoelectron directions for PrIr2Zn20 are reproduced by theoretical analysis for the Gamma_3 ground state, whereas those of the Pr 3d and 4d core levels indicate the Gamma_5 ground state for PrB6., Comment: 6 pages, 4 figures

We have developed a polarized hard X-ray photoemission (HAXPES) system to study the ground-state symmetry of strongly correlated materials. The linear polarization of the incoming X-ray beam is switched by the transmission-type phase retarder composed of two diamond (100) crystals. The best degree of the linear polarization $P_L$ is $-0.96$, containing the vertical polarization component of 98%. A newly developed low temperature two-axis manipulator enables easy polar and azimuthal rotations to select the detection direction of photoelectrons. The lowest temperature achieved is 9 K, offering us a chance to access the ground state even for the strongly correlated electron systems in cubic symmetry. The co-axial sample monitoring system with the long-working-distance microscope enables us to keep measuring the same region on the sample surface before and after rotation procedures. Combining this sample monitoring system with a micro-focused X-ray beam by means of an ellipsoidal Kirkpatrick-Baez mirror (25 $\mu$m $\times$ 25 $\mu$m (FWHM)), we have demonstrated the polarized valence-band HAXPES on NiO for voltage application as resistive random access memories to reveal the origin of the metallic spectral weight near the Fermi level., Comment: to be published in Review of Scientific Instruments

We have successfully observed linear dichroism in angle-resolved Yb3+ 3d5/2 core-level photoemission spectra for YbB12 in cubic symmetry. Its anisotropic 4f charge distribution due to the crystal-field splitting is responsible for the linear dichroism, which has been verified by spectral simulations using ionic calculations with the full multiplet theory for a single-site Yb3+ ion in cubic symmetry. The observed linear dichroism as well as the polarization-dependent spectra in two different photoelectron directions for YbB12 are quantitatively reproduced by theoretical analysis for the Gamma_8 ground state, indicating the Gamma_8 ground-state symmetry for the Yb3+ ions mixed with the Yb2+ state., Comment: 5 pages, 3 figures, to be published in J. Phys. Soc. Jpn. (Letters)

We show that the strongly correlated 4f-orbital symmetry of the ground state is revealed by linear dichroism in core-level photoemission spectra as we have discovered for YbRh2Si2 and YbCu2Si2. Theoretical analysis tells us that the linear dichroism reflects the anisotropic charge distributions resulting from crystalline electric field. We have successfully determined the ground-state 4f symmetry for both compounds from the polarization-dependent angle-resolved core-level spectra at a low temperature well below the first excitation energy. The excited-state symmetry is also probed by temperature dependence of the linear dichroism where the high measuring temperatures are of the order of the crystal-field-splitting energies., Comment: 6 pages, 4 figures, to be published in J. Phys. Soc. Jpn. (Letters)

We present genuine bulk Ir 5d jeff states of layered perovskite iridates obtained by hard-x-ray photoemission spectroscopy (HAXPES) with s- and p-polarized lights. HAXPES spectra of Sr2IrO4 and Ba2IrO4 are well reproduced by the quasi-particle densities of states calculated by the local density approximation with dynamical mean-field theory (LDA+DMFT). It is demonstrated that the insulating nature of the iridates is triggered by antiferromagnetic correlation (Slater type) combined with electron correlation (Mott type). The extremely-low-energy bulk-sensitive photoemission spectroscopy reveals "bad metallic" states in the paramagnetic phase of the iridates, suggesting strongly renormalized metallic states above the Neel temperature as predicted by the LDA+DMFT., Comment: 5 pages, 3 figures

Bulk-sensitive hard x-ray photoemission spectroscopy (HAXPES) reveals for as-grown epitaxial films of half-metallic ferromagnetic CrO2(100) a pronounced screening feature in the Cr 2p3/2 core level and an asymmetry in the O 1s core level. This gives evidence of a finite, metal-type Fermi edge, which is surprisingly not observed in HAXPES. A spectral weight shift in HAXPES away from the Fermi energy is attributed to single-ion recoil effects due to high energy photoelectrons. In conjunction with inverse PES the intrinsic correlated Mott-Hubbard-type electronic structure is unravelled, yielding an averaged Coulomb correlation energy Uav ~ 3.2 eV., Comment: Manuscript 12 pages, 4 figures; Supplemental material 7 pages, 5 figures

We have investigated the electronic structures of recently discovered superconductor FeSe by soft-x-ray and hard-x-ray photoemission spectroscopy with high bulk sensitivity. The large Fe 3d spectral weight is located in the vicinity of the Fermi level (EF), which is demonstrated to be a coherent quasi-particle peak. Compared with the results of the band structure calculation with local-density approximation, Fe 3d band narrowing and the energy shift of the band toward EF are found, suggesting an importance of the electron correlation effect in FeSe. The self energy correction provides the larger mass enhancement value (Z^-1=3.6) than in Fe-As superconductors and enables us to separate a incoherent part from the spectrum. These features are quite consistent with the results of recent dynamical mean-field calculations, in which the incoherent part is attributed to the lower Hubbard band., Comment: 8 pages, 5 figures, 1 talble

We have examined the valence-band electronic structures of gold and silver in the same column in the periodic table with nominally filled d orbitals by means of a recently developed polarization-dependent hard x-ray photoemission. Contrary to a common expectation, it is found that the 5d-orbital electrons contribute prominently to the conduction electrons in gold while the conduction electrons in silver are to some extent free-electron-like with negligible 4d contribution, which could be related to a well-known fact that gold is more stable than silver in air. The 4d electron correlation effects are found to be essential for the conduction electron character in silver., Comment: 8 pages, 4 figures, to be appeared in New J. Phys.

Hard X-ray and extremely low energy bulk-sensitive photoelectron spectroscopy has been performed in the temperature range of 100-330 K for Fe3O4. In the high temperature phase just above the Verwey transition, the intensity at the Fermi level (EF) is still negligible, but it increases gradually with further increasing the temperature (250 K, 330 K) in consistence with the temperature dependence of the conductivity. The spectral behaviors near EF with temperature are well explained by the model, which takes the polaron effect into account., Comment: 5 pages, 3 figures

Dependence of the spectral functions on temperature and rare-earth substitution was examined in detail for Kondo semiconductor alloys Sm1-xEuxB6 and Yb1-xLuxB12 by bulk-sensitive photoemission. It is found that the 4f lattice coherence and intrinsic (small) energy gap are robust for SmB6 against the Eu substitution up to x = 0.15 while both collapse by Lu substitution already at x = 0.125 for YbB12. Our results suggest that the mechanism of the intrinsic gap formation is different between SmB6 and YbB12 although they were so far categorized in the same kind of Kondo semiconductors., Comment: 5 pages, 3 figures

We have performed high-resolution hard X-ray photoemission spectroscopy for the metal-insulator transition (MIT) system (V(1-x)Cr(x))2O3 in the paramagnetic metal, paramagnetic insulator and antiferromagentic insulator phases. The quality of the spectra enables us to conclude that the on-site Coulomb energy U does not change through the MIT, which eliminate all but one theoretical MIT scenario in this paradigm material., Comment: 4 pages, 3 figures

Soft and hard X-ray photoelectron spectroscopy (PES) has been performed for one of the heavy fermion system CeRu$_2$Si$_2$ and a $4f$-localized ferromagnet CeRu$_2$Ge$_2$ in the paramagnetic phase. The three-dimensional band structures and Fermi surface (FS) shapes of CeRu$_2$Si$_2$ have been determined by soft X-ray $h\nu$-dependent angle resolved photoelectron spectroscopy (ARPES). The differences in the Fermi surface topology and the non-$4f$ electronic structures between CeRu$_2$Si$_2$ and CeRu$_2$Ge$_2$ are qualitatively explained by the band-structure calculation for both $4f$ itinerant and localized models, respectively. The Ce valences in CeRu$_2X_2$ ($X$ = Si, Ge) at 20 K are quantitatively estimated by the single impurity Anderson model calculation, where the Ce 3d hard X-ray core-level PES and Ce 3d X-ray absorption spectra have shown stronger hybridization and signature for the partial $4f$ contribution to the conduction electrons in CeRu$_2$Si$_2$., Comment: 8figures

We report on the Cu 1s resonant inelastic X-ray scattering (RIXS) of Cu-O one-dimensional (1D) strongly correlated insulator systems with contrasting atomic arrangements, namely edge-sharing CuGeO3 and corner-sharing Sr2CuO3. Owing to good statistics of the high-resolution RIXS data, so far unresolved fine structures are revealed. Detailed photon-energy and momentum dependence of the RIXS spectra in comparison with theoretical calculations has clarified the natures of the low-energy charge excitations and hybridization of the electronic states., Comment: 4 pages, 3 color figures

Unusual temperature and doping dependence of the Mn 3d spectral functions of manganese perovskites Nd1-xSrxMnO3 has been revealed by the high-resolution Mn 2p-3d resonance photoemission. The temperature-dependent spectra cannot be explained by any theoretical model currently under debate, while showing evidence for a microscopic and dynamic phase segregation. The experimental results strongly suggest that the competition of both the dynamical and static Jahn-Teller effects with ferromagnetic ordering at high and low temperatures, respectively, is responsible for the actual electronic states., Comment: 4 pages, 2 figures

The resonant inelastic x-ray scattering (RIXS) was measured in an insulating SrCuO$_{2}$ with changing the incident photon energy ($h\nu$) near the Cu $1s$ absorption edge (K-edge). Complex structures and their dependences on the momentum transfer($\Delta k$) and $h\nu$ were observed. The $h\nu$ dependence of the RIXS spectra measured for a constant $\Delta k$=2.4$\pi$ has shown a remarkable enhancement near the absorption maximum and a shift of the spectral weight toward larger loss-energy with increasing $h\nu$. Also, the energy of the inelastic loss peak in the RIXS spectra for the fixed excitation at 8.993 keV, 10 eV below the absorption maximum, has shown a clear dependence on $\Delta k$. These results are in a qualitative agreement with a theoretical prediction. Full utilization of the potential of the high brilliance X ray light source at BL19LXU of SPring-8 with 27 m long insertion device will open up a breakthrough in RIXS for heavy transition metal compounds in accordance with the improvement in focussing and analyzing elements., Comment: 7 pages, 5 figures, jpsj2.cls

High-resolution bulk-sensitive photoemission has been measured for pyrochlore oxide Cd2Re2O7. Temperature variations of the spectral shapes between 20 and 250 K are obviously observed for the Re 4f inner core and the valence band spectra. The Re 5d states are dominant for the DOS near the Fermi level., Comment: 4 pages, 3 ps figures, To appear in proceedings of SCES 2002 (Krakow)