Convergence of quasiparticle self-consistent GW calculations of transition metal monoxides

Abstract

Finding an accurate ab initio approach for calculating the electronic properties of transition metal oxides has been a problem for several decades. In this paper, we investigate the electronic structure of the transition metal monoxides MnO, CoO, and NiO in their undistorted rock-salt structure within a fully iterated quasiparticle self-consistent GW (QPscGW) scheme. We study the convergence of the QPscGW method, i.e., how the quasiparticle energy eigenvalues and wavefunctions converge as a function of the QPscGW iterations, and we compare the converged outputs obtained from different starting wavefunctions. We find that the convergence is slow and that a one-shot G${}_0$W${}_0$ calculation does not significantly improve the initial eigenvalues and states. It is important to notice that in some cases the "path" to convergence may go through energy band reordering which cannot be captured by the simple initial unperturbed Hamiltonian. When we reach a fully iterated solution, the converged density of states, band-gaps and magnetic moments of these oxides are found to be only weakly dependent on the choice of the starting wavefunctions and in reasonably good agreement with the experiment. Finally, this approach provides a clear picture of the interplay between the various orbitals near the Fermi level of these simple transition metal monoxides. The results of these accurate {\it ab initio} calculations can provide input for models aiming at describing the low energy physics in these materials.

arXiv comment14 Latex pages, 10 Figures with multiple subfigures

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• Pressure dependence of dynamically screened Coulomb interactions in NiO: Effective Hubbard, Hund, intershell and intersite components
• Verification of Anderson superexchange in MnO via magnetic pair distribution function analysis and \textit{ab initio} theory
• High photon energy spectroscopy of NiO: experiment and theory
• Influence of magnetic ordering on the spectral properties of binary transition metal oxides
• Variational Excitations in Real Solids: Optical Gaps and Insights into Many-Body Perturbation Theory
• Photoemission spectrum in paramagnetic FeO under pressure: towards an \textit{ab-initio} description
• Towards understanding the electronic structure of the simpler members of two-dimensional halide-perovskites
• Magnetic force theory combined with quasi-particle self-consistent GW method
• Analysis of diagonal G and subspace W approximations within fully self-consistent GW calculations for bulk semiconducting systems
• Excitonic-trion population in two-dimensional halide perovskites
• All-electron Quasiparticle Self-consistent GW for Molecules and Periodic Systems within the Numerical Atomic Orbital Framework