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Register a new userHidden relationship between the electrical conductivity and the Mn 2p core-level photoemission spectra in La1-xSrxMnO3
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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 photoemission 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.
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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.
We have re-examined the valence-band (VB) and core-level electronic structure of NiO by means of hard and soft x-ray photoemission spectroscopy (PES). The spectral weight of the lowest energy state found to be enhanced in the bulk sensitive Ni 2p core-level PES. A configuration-interaction model including the bound state screening has shown significant agreement with the core-level spectra, and the off and on-resonance VB spectra. These results identify the lowest energy state in core-level and VB-PES as the Zhang-Rice doublet bound state, consistent with the spin-fermion model and recent ab initio calculation with dynamical mean-field theory (LDA + DMFT).
We have performed a detailed study of Cu $2p$ core-level spectra in single layer La$_{2-x}$Sr$_{x}$CuO$_{4}$, La doped Bi$_2$Sr$_{1.6}$La$_{0.4}$CuO$_{6+delta}$ (Bi2201) and bilayer Bi$_2$Sr$_{2}$CaCu$_{2}$O$_{8+delta}$ (Bi2212) high-temperature superconductors by using hard x-ray photoemission (HX-PES). We identify the Cu$^{2+}$ derived (i) the Zhang-Rice singlet (ZRS) feature, (ii) the $d^{n+1}underline{L}$ (ligand screened) feature, (iii) the $d^{n}$ satellite feature, as well as the hole-doping derived high binding energy feature in the main peak. In Bi-based cuprates, intensities of the $d^{n}$ satellite features seem to be strongly enhanced compared to La$_{2-x}$Sr$_{x}$CuO$_{4}$. From x-ray photon energy dependent measurements, it is shown that the increased intensity in the satellite region is associated with Bi $4s$ core-level spectral intensity. The corrected $d^{n}$ satellite intensity is independent of the doping content or number of Cu-O layers. Our results suggest a correlation of the relative intensity of ZRS feature and hole-doping induced high binding energy spectral changes in the main peak with superconductivity.
We have explored spin, charge and orbitally ordered states in La1-xSrxMnO3 (0 < x < 1/2) using model Hartree-Fock calculations on d-p-type lattice models. At x=1/8, several charge and orbitally modulated states are found to be stable and almost degenerate in energy with a homogeneous ferromagnetic state. The present calculation indicates that a ferromagnetic state with a charge modulation along the c-axis which is consistent with the experiment by Yamada et al. might be responsible for the anomalous behavior around x = 1/8.
We report on the pressure effects on the orbital polaron lattice in the lightly doped manganites $mathrm{La_{1-x}Sr_xMnO_{3}}$, with $xsim 1/8$. The dependence of the orbital polaron lattice on $negative$ chemical pressure is studied by substituting Pr for La in $mathrm{(La_{1-y}Pr_y)_{7/8}Sr_{1/8}MnO_{3}}$. In addition, we have studied its hydrostatic pressure dependence in $mathrm{(La_{0.9}Pr_{0.1})_{7/8}Sr_{1/8}MnO_{3}}$. Our results strongly indicate that the hopping $t$ significantly contributes to the stabilization of the orbital polaron lattice and that the orbital polarons are ferromagnetic objects which get stabilized by local double exchange processes. The analysis of short range orbital correlations and the verification of the Grueneisen scaling by hard x-ray, specific heat and thermal expansion data reinforces our conclusions.
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