Accurate optical spectra of solids from pure time-dependent density-functional theory

Abstract

We present accurate optical spectra of semiconductors and insulators within a pure Kohn-Sham time-dependent density-functional approach. In particular, we show that the onset of the absorption is well reproduced when comparing to experiment. No empirical information nor a theory beyond Kohn-Sham density-functional theory, such as $GW$, is invoked to correct the Kohn-Sham gap. Our approach relies on the link between the exchange-correlation kernel of time-dependent density functional theory and the derivative discontinuity of ground-state density-functional theory. We show explicitly how to relate these two quantities. We illustrate the accuracy and simplicity of our approach by applying it to various semiconductors (Si, GaP, GaAs) and wide-gap insulators (C, LiF, Ar).

arXiv comment7 pages, 6 figures

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• A Snapshot of Time-Dependent Density-Functional Theory
• Accurate and efficient prediction of the band gaps and optical spectra of chalcopyrite semiconductors from a non-empirical range-separated dielectric-dependent hybrid: Comparison with many-body perturbation theory
• Exact exchange-correlation potentials for calculating the fundamental gap with a fixed number of electrons
• Optical spectra of 2D monolayers from time-dependent density functional theory
• Excitonic effects in time-dependent density functional theory from zeros of the density response
• Wigner-Seitz truncated TDDFT approach for the calculation of exciton binding energies in solids
• Exact expressions for the height of the interatomic step in the exchange-correlation potential from the derivative discontinuity of the energy