Converged GW quasiparticle energies for transition metal oxide perovskites

Abstract

The ab initio calculation of quasiparticle (QP) energies is a technically and computationally challenging problem. In condensed matter physics the most widely used approach to determine QP energies is the GW approximation. Although the GW method has been widely applied to many typical semiconductors and insulators, its application to more complex compounds such as transition metal oxide perovskites has been comparatively rare, and its proper use is not well established from a technical point of view. In this work, we have applied the single-shot G0W0 method to a representative set of transition metal oxide perovskites including 3d (SrTiO3, LaScO3, SrMnO3, LaTiO3, LaVO3, LaCrO3, LaMnO3, and LaFeO3), 4d (SrZrO3, SrTcO3, and Ca2RuO4) and 5d (SrHfO3, KTaO3 and NaOsO3) compounds with different electronic configurations, magnetic orderings, structural characteristics and bandgaps ranging from 0.1 to 6.1 eV. We discuss the proper procedure to obtain well converged QP energies and accurate bandgaps within single-shot G0W0 by comparing the conventional approach based on an incremental variation of a specific set of parameters (number of bands, energy cutoff for the plane-wave expansion and number of k-points and the basis-set extrapolation scheme [Phys. Rev. B 90, 075125 (2014)]. In addition, we have inspected the difference between the adoption of norm-conserving and ultrasoft potentials in GW calculations. A minimal statistical analysis indicates that the correlation of the GW data with the DFT gap is more robust than the correlation with the experimental gaps; moreover we identify the static dielectric constant as alternative useful parameter for the approximation of GW gap in high-throughput automatic procedures. Finally, we compute the QP band structure and spectra within the random phase approximation and compare the results with available experimental data.

arXiv commentPhysical Review Materials, accepted

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• Vertex corrections to the polarizability do not improve the GW approximation for the ionization potential of molecules
• Strain-induced tuning of the electronic Coulomb interaction in 3d transition metal oxide perovskites
• Electron correlations in cubic paramagnetic perovskite Sr(V,Mn)O${}_3$ -- Results from fully self-consistent self-energy embedding calculations
• Comparative ab initio study of the structural, electronic, magnetic, and dynamical properties of LiOsO${}_3$ and NaOsO${}_3$
• Many-body electronic structure of LaScO${}_3$ by real space quantum Monte Carlo
• Exploring the role of nonlocal Coulomb interactions in perovskite transition metal oxides
• Superconductivity in SrTiO${}_3$: dielectric function method for non-parabolic bands
• Landscape of coexisting excitonic states in the insulating single-layer cuprates and nickelates
• Embedding vertex corrections in GW self-energy: theory, implementation, and outlook
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