Abstract:Orbital ordering has been less investigated in epitaxial thin films, due to the difficulty to evidence directly the occurrence of this phenomenon in thin film samples. Atomic resolution electron microscopy enabled us to observe the structural details of the ultrathin LaVO3 films. The transition to orbital ordering of epitaxial layers as thin as ≈4 nm was probed by temperature‐dependent Raman scattering spectroscopy of multilayer samples. From the occurrence and temperature dependence of the 700 cm–1 Raman acti… Show more
“…,Lu, which reveal temperature-induced magnetization reversals [41] as a result of the coupling of spin and orbital degrees of freedom of the t 2g valence electrons [42][43][44][45][46][47]. This class of compounds has interesting phase diagrams with two complementary spinorbital ordered phases and a pure orbital-ordered phase [48][49][50][51][52][53][54]. Remarkably, the C-type spin and G-type orbital ordered phase in La 1−x Sr x VO 3 , Pr 1−x Ca x VO 3 and Y 1−x Ca x VO 3 is robust up to high-doping concentrations and also the metalinsulator transition takes place only at quite substantial doping [55][56][57][58].…”
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−xCaxVO3 perovskites, where R = La, . . . , Lu. A fundamental characteristic of these vanadium d 2 compounds with partly filled t2g valence orbitals is the persistence of spin and orbital order up to high doping, in contrast to the loss of magnetic order in high-Tc cuprates at low defect concentration. We demonstrate that the disordered electronic structure of doped Mott-Hubbard insulators can be obtained with high precision within the unrestricted Hartree-Fock approximation. In particular: (i) the atomic multiplet excitations in the inverse photoemission spectra and the various defect-related states and satellites are 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, that 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. We demonstrate that charge defects trigger small spinorbital polarons, with their internal kinetic energy responsible for the opening of the soft defect states gap. This kinetic gap survives disorder fluctuations of defects and is amplified by the long-range e-e interactions, whereas in the atomic limit we observe a Coulomb singularity. The small size of spin-orbital polarons is inferred by an analysis of the inverse participation ratio which explains the origin of the robustness of spin and orbital order. Using realistic parameters for the perovskite vanadate system La1−xCaxVO3, we show that its soft gap is well 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.
“…,Lu, which reveal temperature-induced magnetization reversals [41] as a result of the coupling of spin and orbital degrees of freedom of the t 2g valence electrons [42][43][44][45][46][47]. This class of compounds has interesting phase diagrams with two complementary spinorbital ordered phases and a pure orbital-ordered phase [48][49][50][51][52][53][54]. Remarkably, the C-type spin and G-type orbital ordered phase in La 1−x Sr x VO 3 , Pr 1−x Ca x VO 3 and Y 1−x Ca x VO 3 is robust up to high-doping concentrations and also the metalinsulator transition takes place only at quite substantial doping [55][56][57][58].…”
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−xCaxVO3 perovskites, where R = La, . . . , Lu. A fundamental characteristic of these vanadium d 2 compounds with partly filled t2g valence orbitals is the persistence of spin and orbital order up to high doping, in contrast to the loss of magnetic order in high-Tc cuprates at low defect concentration. We demonstrate that the disordered electronic structure of doped Mott-Hubbard insulators can be obtained with high precision within the unrestricted Hartree-Fock approximation. In particular: (i) the atomic multiplet excitations in the inverse photoemission spectra and the various defect-related states and satellites are 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, that 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. We demonstrate that charge defects trigger small spinorbital polarons, with their internal kinetic energy responsible for the opening of the soft defect states gap. This kinetic gap survives disorder fluctuations of defects and is amplified by the long-range e-e interactions, whereas in the atomic limit we observe a Coulomb singularity. The small size of spin-orbital polarons is inferred by an analysis of the inverse participation ratio which explains the origin of the robustness of spin and orbital order. Using realistic parameters for the perovskite vanadate system La1−xCaxVO3, we show that its soft gap is well 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.
“…Experimentally, this was examined in high-pressure studies, which showed that the ground state of RVO 3 can be altered under sufficient pressure [43][44][45]. This lattice coupling was also inspected in thin films of LaVO 3 [46][47][48][49] and PrVO 3 [50,51], where biaxial epitaxial strain was utilized to modify their ordering temperatures.…”
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