Spin-state transition and spin-polaron physics in cobalt oxide perovskites: ab initio approach based on quantum chemical methods

Abstract

A fully ab initio scheme based on quantum chemical wavefunction methods is used to investigate the correlated multiorbital electronic structure of a 3d-metal compound, LaCoO3. The strong short-range electron correlations, involving both Co and O orbitals, are treated by multireference techniques. The use of effective parameters like the Hubbard U and interorbital U', J terms and the problems associated with their explicit calculation are avoided with this approach. We provide new insight into the spin-state transition at about 90 K and the nature of charge carriers in the doped material. Our results indicate the formation of a t4e2 high-spin state in LaCoO3 for T>90 K. Additionally, we explain the paramagnetic phase in the low-temperature lightly doped compound through the formation of Zhang-Rice-like O hole states and ferromagnetic clusters.

References in corpus (14)

• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• Quantum Cluster Theories
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• The spin state transition in LaCoO${}_3$; revising a revision
• Structural phenomena associated with the spin-state transition in LaCoO3
• Evidence for orbital ordering in LaCoO3
• Spin-state transition in LaCoO3: direct neutron spectroscopic evidence of excited magnetic states
• Strain-induced insulator state in La_0.7Sr_0.3CoO_3
• Screening of Coulomb interactions in transition metals
• Obtaining Wannier Functions of a Crystalline Insulator within a Hartree-Fock approach: Applications to LiF and LiCl
• Fermiology of Cuprates from First Principles: From Small Pockets to the Luttinger Fermi surface
• A simplified method for the computation of correlation effects on the band structure of semiconductors
• Ab initio wavefunction based methods for excited states in solids: correlation corrections to the band structure of ionic oxides
• Quasiparticle bands in cuprates by quantum chemical methods: towards an ab initio description of strong electron correlations

Cited by in corpus (16)

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• Lattice structure and magnetization of LaCoO3 thin films
• Quasi-2D magnetic correlations in Ni${}_2$P${}_2$S${}_6$ probed by ${}^{31}$P NMR
• Correlated electrons in Fe-As compounds: a quantum chemical perspective
• Correlation-induced corrections to the band structure of boron nitride: a wave-function-based approach
• Ab initio computation of d-d excitation energies in low-dimensional Ti and V oxychlorides
• The effect of different in-chain impurities on the magnetic properties of the spin chain compound SrCuO${}_2$ probed by NMR
• Resonating holes vs molecular spin-orbit coupled states in group-5 lacunar spinels
• Wave-function-based approach to quasiparticle bands: new insight into the electronic structure of c-ZnS
• Crystal-field effects competing with spin-orbit interactions in NaCeO${}_2$
• Quantum chemical insights into hexaboride electronic structures: correlations within the boron $p$-orbital subsystem
• Yb${}^{3+}$ $f$-$f$ excitations in NaYbSe${}_2$: benchmarking embedded-cluster quantum chemical schemes for 4$f$ insulators
• Relevance of on-site and intersite Coulomb interactions in the Kitaev-Heisenberg magnet Na${}_3$Co${}_2$SbO${}_6$