Optical properties of correlated materials: Generalized Peierls approach and its application to VO2

The aim of this paper is to present a versatile scheme for the computation of optical properties of solids, with particular emphasis on realistic many-body calculations for correlated materials. Geared at the use with localized basis sets, we extend the commonly known lattice Peierls substitution approach to the case of multiatomic unit cells. We show in how far this generalization can be deployed as an approximation to the full Fermi-velocity matrix elements that enter the continuum description of the response of a solid to incident light. We further devise an upfolding scheme to incorporate optical transitions that involve high-energy orbitals that had been downfolded in the underlying many-body calculation of the electronic structure. As an application of the scheme, we present results on a material of longstanding interest, vanadium dioxide, VO2. Using dynamical mean-field data of both, the metallic and the insulating phase, we calculate the corresponding optical conductivities, elucidate optical transitions and find good agreement with experimental results.