Orbital-resolved DFT+U for molecules and solids

Abstract

We present an orbital-resolved extension of the Hubbard $U$ correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly improved, particularly for compounds characterized by both localized and hybridized states in the Hubbard manifold. The numerical values of all Hubbard parameters are readily obtained from linear-response calculations. The relevance of this more refined approach is showcased by its application to bulk solids pyrite (FeS${}_2$) and pyrolusite ($\beta$-MnO${}_2$), as well as to six Fe(II) molecular complexes. Our findings indicate that a careful definition of Hubbard manifolds is indispensable for extending the applicability of DFT+$U$ beyond its current boundaries. The present orbital-resolved scheme aims to provide a computationally undemanding yet accurate tool for electronic structure calculations of charge-transfer insulators, transition-metal (TM) complexes and other compounds displaying significant orbital hybridization.

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• Explicit demonstration of the equivalence between DFT+U and the Hartree-Fock limit of DFT+DMFT
• First-principles Hubbard parameters with automated and reproducible workflows
• Magnons from time-dependent density-functional perturbation theory and nonempirical Hubbard functionals
• Comparative analysis of methods for calculating Hubbard parameters using cRPA
• Comparative study of magnetic exchange parameters and magnon dispersions in NiO and MnO from first principles
• Flat-plane based double-counting free and parameter free many-body DFT+U
• A method to derive material-specific spin-bath model descriptions of materials displaying prevalent spin physics
• Getting the manifold right: The crucial role of orbital resolution in DFT+U for mixed d-f electron compounds
• Bridging constrained random-phase approximation and linear response theory for computing Hubbard parameters