Linear response time-dependent density functional theory without unoccupied states: The Kohn-Sham-Sternheimer scheme revisited

The Journal of Chemical Physics
Fabian HofmannStephan Kümmel

Abstract

The Sternheimer approach to time-dependent density functional theory in the linear response regime is attractive because of its computational efficiency. The latter results from avoiding the explicit calculation of unoccupied orbitals and from the basic structure of the Sternheimer equations, which naturally lend themselves to far-reaching parallelization. In this article, we take a fresh look at the frequency-dependent Sternheimer equations. We first give a complete, self-contained derivation of the equations that complements previous derivations. We then discuss several aspects of an efficient numerical realization. As a worked example, we compute the photoabsorption spectra of small hydrogenated silicon clusters and confirm that for these the quality of the Kohn-Sham eigenvalues is more important than the effects of the exchange-correlation kernel. Finally, we demonstrate how triplet excitations can readily be computed from the Sternheimer approach.

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Citations

Sep 24, 2020·The Journal of Chemical Physics·Fabian Hofmann, Stephan Kümmel
Sep 7, 2020·The Journal of Chemical Physics·Johannes Flick, Prineha Narang
Aug 18, 2021·The Journal of Physical Chemistry. a·Giulia GiannoneFabio Della Sala

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