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Register a new userOn the effect of charge self-consistency in DFT+DMFT calculations for complex transition metal oxides
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We investigate the effect of charge self-consistency (CSC) in density functional theory plus dynamical mean-field theory (DFT+DMFT) calculations compared to simpler one-shot calculations for materials where interaction effects lead to a strong redistribution of electronic charges between different orbitals or between different sites. We focus on two systems close to a metal-insulator transition, for which the importance of CSC is currently not well understood. Specifically, we analyze the strain-related orbital polarization in the correlated metal CaVO$_3$ and the spontaneous electronic charge disproportionation in the rare-earth nickelate LuNiO$_3$. In both cases, we find that the CSC treatment reduces the charge redistribution compared to cheaper one-shot calculations. However, while the MIT in CaVO$_3$ is only slightly shifted due to the reduced orbital polarization, the effect of the site polarization on the MIT in LuNiO$_3$ is more subtle. Furthermore, we highlight the role of the double-counting correction in CSC calculations containing different inequivalent sites.
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We investigate the dispersion of the charge carrier plasmon in the three prototypical charge-density wave bearing transition-metal dichalcogenides 2H-TaSe2, 2H-TaS2 and 2H-NbSe2 employing electron energy-loss spectroscopy. For all three compounds the plasmon dispersion is found to be negative for small momentum transfers. This is in contrast to the generic behavior observed in simple metals as well as the related system 2H-NbS2, which does not exhibit charge order. We present a semiclassical Ginzburg-Landau model which accounts for these observations, and argue that the vicinity to a charge ordered state is thus reflected in the properties of the collective excitations.
We discuss the recently proposed LDA+DMFT approach providing consistent parameter free treatment of the so called double counting problem arising within the LDA+DMFT hybrid computational method for realistic strongly correlated materials. In this approach the local exchange-correlation portion of electron-electron interaction is excluded from self consistent LDA calculations for strongly correlated electronic shells, e.g. d-states of transition metal compounds. Then the corresponding double counting term in LDA+DMFT Hamiltonian is consistently set in the local Hartree (fully localized limit - FLL) form of the Hubbard model interaction term. We present the results of extensive LDA+DMFT calculations of densities of states, spectral densities and optical conductivity for most typical representatives of two wide classes of strongly correlated systems in paramagnetic phase: charge transfer insulators (MnO, CoO and NiO) and strongly correlated metals (SrVO3 and Sr2RuO4). It is shown that for NiO and CoO systems LDA+DMFT qualitatively improves the conventional LDA+DMFT results with FLL type of double counting, where CoO and NiO were obtained to be metals. We also include in our calculations transition metal 4s-states located near the Fermi level missed in previous LDA+DMFT studies of these monooxides. General agreement with optical and X-ray experiments is obtained. For strongly correlated metals LDA$^prime$+DMFT results agree well with earlier LDA+DMFT calculations and existing experiments. However, in general LDA+DMFT results give better quantitative agreement with experimental data for band gap sizes and oxygen states positions, as compared to the conventional LDA+DMFT.
We show that a class of compounds with $I$4/$mcm$ crystalline symmetry hosts three-dimensional semi-Dirac fermions. Unlike the known two-dimensional semi-Dirac points, the degeneracy of these three-dimensional semi-Dirac points is not lifted by spin-orbit coupling due to the protection by a nonsymmorphic symmetry -- screw rotation in the $a-b$ plane and a translation along the $c$ axis. This crystalline symmetry is found in tetragonal perovskite oxides, realizable in thin films by epitaxial strain that results in a$^0$a$^0$c$^-$-type octahedral rotation. Interestingly, with broken time-reversal symmetry, two pairs of Weyl points emerge from the semi-Dirac points within the Brillouin zone, and an additional lattice distortion leads to enhanced intrinsic anomalous Hall effect. We discuss possible fingerprints of this symmetry-protected band topology in electronic transport experiments.
Magnetism of transition metal (TM) oxides is usually described in terms of the Heisenberg model, with orientation-independent interactions between the spins. However, the applicability of such a model is not fully justified for TM oxides because spin polarization of oxygen is usually ignored. In the conventional model based on the Anderson principle, oxygen effects are considered as a property of the TM ion and only TM interactions are relevant. Here, we perform a systematic comparison between two approaches for spin polarization on oxygen in typical TM oxides. To this end, we calculate the exchange interactions in NiO, MnO, and hematite (Fe2O3) for different magnetic configurations using the magnetic force theorem. We consider the full spin Hamiltonian including oxygen sites, and also derive an effective model where the spin polarization on oxygen renormalizes the exchange interactions between TM sites. Surprisingly, the exchange interactions in NiO depend on the magnetic state if spin polarization on oxygen is neglected, resulting in non-Heisenberg behavior. In contrast, the inclusion of spin polarization in NiO makes the Heisenberg model more applicable. Just the opposite, MnO behaves as a Heisenberg magnet when oxygen spin polarization is neglected, but shows strong non-Heisenberg effects when spin polarization on oxygen is included. In hematite, both models result in non-Heisenberg behavior. General applicability of the magnetic force theorem as well as the Heisenberg model to TM oxides is discussed.
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