Subspace representations in ab initio methods for strongly correlated systems

Abstract

We present a generalized definition of subspace occupancy matrices in ab initio methods for strongly correlated materials, such as DFT+U and DFT+DMFT, which is appropriate to the case of nonorthogonal projector functions. By enforcing the tensorial consistency of all matrix operations, we are led to a subspace projection operator for which the occupancy matrix is tensorial and accumulates only contributions which are local to the correlated subspace at hand. For DFT+U in particular, the resulting contributions to the potential and ionic forces are automatically Hermitian, without resort to symmetrization, and localized to their corresponding correlated subspace. The tensorial invariance of the occupancies, energies and ionic forces is preserved. We illustrate the effect of this formalism in a DFT+U study using self-consistently determined projectors.

15 pages, 8 figures. This version (v2) matches that accepted for Physical Review B on 15th April 2011

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• Theory of projections with non-orthogonal basis sets: Partitioning techniques and effective Hamiltonians
• Renormalization of myoglobin-ligand binding energetics by quantum many-body effects
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• Wannier-function-based constrained DFT with nonorthogonality-correcting Pulay forces in application to the reorganization effects in graphene-adsorbed pentacene
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