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A laboratory hard X-ray photoelectron spectroscopy (HXPS) system equipped with a monochromatic Cr K$alpha$ ($h u = 5414.7$ eV) X-ray source was applied to an investigation of the core-level electronic structure of La$_{1-x}$Sr$_x$MnO$_3$. No apprecia ble high binding-energy shoulder in the O $1s$ HXPS spectra were observed while an enhanced low binding-energy shoulder structure in the Mn $2p_{3/2}$ HXPS spectra were observed, both of which are manifestation of high bulk sensitivity. Such high bulk sensitivity enabled us to track the Mn $2p_{3/2}$ shoulder structure in the full range of $x$, giving us a new insight into the binding-energy shift of the Mn $2p_{3/2}$ core level. Comparisons with the results using the conventional laboratory XPS ($h u = 1486.6$ eV) as well as those using a synchrotron radiation source ($h u = 7939.9$ eV) demonstrate that HXPS is a powerful and convenient tool to analyze the bulk electronic structure of a host of different compounds.
A detailed low-energy electronic structure of a Kondo insulator YbB$_{12}$ was revealed by a synergetic combination of ultrahigh-resolution laser photoemission spectroscopy (PES) and time-resolved PES. The former confirmed a 25-meV pseudogap correspo nding to the Kondo temperature of this material, and more importantly, it revealed that a 15-meV gap and a Kondo-peak feature developed below a crossover temperature $T^ast sim 110$ K. In harmony with this, the latter discovered a very long recombination time exceeding 100 ps below $sim$$T^ast$. This is a clear manifestation of photoexcited carriers due to the bottleneck in the recovery dynamics, which is interpreted as a developing hybridization gap of a hard gap.
By using laboratory x-ray photoemission spectroscopy (XPS) and hard x-ray photoemission spectroscopy (HX-PES) at a synchrotron facility, we report an empirical semi-quantitative relationship between the valence/core-level x-ray photoemission spectral weight and electrical conductivity in La_{1-x}Sr_{x}MnO_{3} as a function of x. In the Mn 2p_{3/2} HX-PES spectra, we observed the shoulder structure due to the Mn^{3+} well-screened state. However, the intensity at x=0.8 was too small to explain its higher electrical conductivity than x=0.0, which confirms our recent analysis on the Mn 2p_{3/2} XPS spectra. The near-Fermi level XPS spectral weight was found to be a measure of the variation of electrical conductivity with x in spite of a far lower energy resolution compared with the energy scale of the quasiparticle (coherent) peak because of the concurrent change of the coherent and incoherent spectral weight.
Core-level electronic structure of La1-xSrxMnO3 has been studied by x-ray photoemission spectroscopy (XPS). We first report, by the conventional XPS, the well-screened shoulder structure in Mn 2p3/2 peak, which had been observed only by hard x-ray ph otoemission spectroscopy so far. Multiple-peak analysis revealed that the Mn4+ spectral weight was not proportional to the nominal hole concentration x, indicating that a simple Mn3+/Mn4+ intensity ratio analysis may result in a wrong quantitative elemental analysis. Considerable weight of the shoulder at x=0.0 and the fact that the shoulder weight was even slightly going down from x=0.2 to 0.4 were not compatible with the idea that this weight simply represents the metallic behavior. Further analysis found that the whole Mn 2p3/2 peak can be decomposed into four portions, the Mn4+, the (nominal) Mn3+, the shoulder, and the other spectral weight located almost at the Mn3+ location. We concluded that this weight represents the well-screened final state at Mn4+ sites, whereas the shoulder is known as that of the Mn3+ states. We found that the sum of these two spectral weight has an empirical relationship to the conductivity evolution with x.
We report the detailed electronic structure of a hole-doped delafossite oxide CuCr_{1-x}Mg_{x}O_{2} (0 <= x <= 0.03) studied by photoemission spectroscopy (PES), soft x-ray absorption spectroscopy (XAS), and band-structure calculations within the loc al-density approximation +U (LDA+U) scheme. Cr/Cu 3p-3d resonant PES reveals that the near-Fermi-level leading structure has primarily the Cr 3d character with a minor contribution from the Cu 3d through Cu 3d-O 2p-Cr 3d hybridization, having good agreement with the band-structure calculations. This indicates that a doped hole will have primarily the Cr 3d character. Cr 2p PES and L-edge XAS spectra exhibit typical Cr^{3+} features for all x, while the Cu L-edge XAS spectra exhibited a systematic change with x. This indicates now that the Cu valence is monovalent at x=0 and the doped hole should have Cu 3d character. Nevertheless, we surprisingly observed two types of charge-transfer satellites that should be attributed to Cu^{+} (3d^{10}) and Cu^{2+} (3d^{9}) like initial states in Cu 2p-3d resonant PES spectrum for at x=0, while Cu 2p PES spectra with no doubt shows the Cu^{+} character even for the lightly doped samples. We propose that these contradictory results can be understood by introducing no only the Cu 4s state, but also finite Cu 3d,4s-Cr 3d charge transfer via O 2p states in the ground-state electronic configuration.
Electronic structures of the quantum critical superconductor beta-YbAlB4 and its polymorph alpha-YbAlB4 are investigated by using bulk-sensitive hard x-ray photoemission spectroscopy. From the Yb 3d core level spectra, the values of the Yb valence ar e estimated to be ~2.73 and ~2.75 for alpha- and beta-YbAlB4, respectively, thus providing clear evidence for valence fluctuations. The valence band spectra of these compounds also show Yb2+ peaks at the Fermi level. These observations establish an unambiguous case of a strong mixed valence at quantum criticality for the first time among heavy fermion systems, calling for a novel scheme for a quantum critical model beyond the conventional Doniach picture in beta-YbAlB4.
Low energy electronic structure of optimally doped YBa2Cu3O7-d is investigated using laser-excited angle-resolved photoemission spectroscopy. The surface state and the CuO chain band that usually overlap the CuO2 plane derived bands are not detected, thus enabling a clear observation of the bulk superconducting state. The observed bilayer splitting of the Fermi surface is ~0.08 angstrom^{-1} along the (0,0)-(pi,pi) direction, significantly larger than Bi2Sr2CaCu2O8+d. The kink structure of the band dispersion reflecting the renormalization effect at ~60 meV shows up similarly as in other hole-doped cuprates. The momentum-dependence of the superconducting gap shows d_{x^2-y^2}-wave like amplitude, but exhibits a nonzero minimum of ~12 meV along the (0,0)-(pi,pi) direction. Possible origins of such an unexpected nodeless gap behavior are discussed.
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