Beyond time-dependent exact exchange: the need for long-range correlation

The Journal of Chemical Physics
Fabien BrunevalLucia Reining

Abstract

In the description of the interaction between electrons beyond the classical Hartree picture, bare exchange often yields a leading contribution. Here we discuss its effect on optical spectra of solids, comparing three different frameworks: time-dependent Hartree-Fock, a recently introduced combined density-functional and Green's function approaches applied to the bare exchange self-energy, and time-dependent exact exchange within time-dependent density-functional theory (TD-EXX). We show that these three approximations give rise to identical excitonic effects in solids; these effects are drastically overestimated for semiconductors. They are partially compensated by the usual overestimation of the quasiparticle band gap within Hartree-Fock. The physics that lacks in these approaches can be formulated as screening. We show that the introduction of screening in TD-EXX indeed leads to a formulation that is equivalent to previously proposed functionals derived from many-body perturbation theory. It can be simulated by reducing the long-range part of the Coulomb interaction: this produces absorption spectra of semiconductors in good agreement with experiment.

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Citations

Jan 26, 2011·The Journal of Chemical Physics·Davide SangalliAndrea Marini
Feb 5, 2009·The Journal of Chemical Physics·P RomanielloG Onida
Jun 17, 2016·The Journal of Chemical Physics·Neepa T Maitra
Sep 24, 2020·The Journal of Chemical Physics·Fabian Hofmann, Stephan Kümmel
Jul 28, 2021·The Journal of Physical Chemistry Letters·Joshua D ElliottPaolo Umari
Apr 19, 2019·Journal of Chemical Theory and Computation·Joshua D ElliottPaolo Umari
Sep 25, 2021·Journal of Chemical Theory and Computation·Xiao Wang, Timothy C Berkelbach

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