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Abstract:
We explore the effects of disordered charged defects on the electronic excitations observed in the photoemission spectra of doped transition metal oxides in the Mott insulating regime by the example of the R1-xCax VO3 perovskites, where R = La,..., Lu. A fundamental characteristic of these vanadium d(2) compounds with partly filled t(2g) valence orbitals is the persistence of spin and orbital order up to high doping, in contrast to the loss of magnetic order in high-T-c cuprates at low defect concentration. We study the disordered electronic structure of such dopedMott-Hubbard insulators within the unrestricted Hartree-Fock approximation and, as a result, manage to explain the spectral features that occur in photoemission and inverse photoemission. In particular, (i) the atomic multiplet excitations in the inverse photoemission spectra and the various defect-related states and satellites are qualitatively well reproduced, (ii) a robust Mott gap survives up to large doping, and (iii) we show that the defect states inside the Mott gap develop a soft gap at the Fermi energy. The soft defect-states gap, which separates the highest occupied from the lowest unoccupied states, can be characterized by a shape and a scale parameter extracted from a Weibull statistical sampling of the density of states near the chemical potential. These parameters provide a criterion and a comprehensive schematization for the insulator-metal transition in disordered systems. Our results provide clear indications that doped holes are bound to charged defects and form small spin-orbital polarons whose internal kinetic energy is responsible for the opening of the soft defect-states gap. We show that this kinetic gap survives disorder fluctuations of defects and is amplified by the long-range electron-electron interactions, whereas we observe a Coulomb singularity in the atomic limit. The small size of spin-orbital polarons is inferred by an analysis of the inverse participation ratio and by means of a complementary many-body polaron theory, which yields a similar robust spin and orbital order as the Hartree-Fock approximation. Using realistic parameters for the vanadium perovskite La1-xCaxVO3, we show that its soft gap is reproduced as well as the marginal doping dependence of the position of the chemical potential relative to the center of the lower Hubbard band. The present theory uncovers also the reasons why the d(1) -> d(0) satellite excitations, which directly probe the effect of the random defect fields on the polaron state, are not well resolved in the available experimental photoemission spectra for La1-xCaxVO3.
