Density-Driven Correlations in Many-Electron Ensembles: Theory and Application for Excited States

Physical Review Letters
Tim Gould, Stefano Pittalis

Abstract

Density functional theory can be extended to excited states by means of a unified variational approach for passive state ensembles. This extension overcomes the restriction of the typical density functional approach to ground states, and offers useful formal and demonstrated practical benefits. The correlation energy functional in the generalized case acquires higher complexity than its ground state counterpart, however. Little is known about its internal structure nor how to effectively approximate it in general. Here we show that such a functional can be broken down into natural components, including what we call "state-" and "density-driven" correlations, with the former amenable to conventional approximations, and the latter being a unique feature of ensembles. Such a decomposition provides us with a pathway to general approximations that are able to routinely handle low-lying excited states. The importance of density-driven correlations is demonstrated, and an approximation for them is introduced and shown to be useful.

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Dec 30, 2017·Physical Review Letters·Tim Gould, Stefano Pittalis
May 10, 2018·The Journal of Chemical Physics·Tim GouldStefano Pittalis
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Oct 8, 2018·The Journal of Chemical Physics·Francisca Sagredo, Kieron Burke

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Citations

Jun 9, 2020·The Journal of Chemical Physics·Pierre-François Loos, Emmanuel Fromager
Dec 19, 2020·Physical Review Letters·Tim GouldStefano Pittalis
Mar 10, 2021·The Journal of Chemical Physics·Tim Gould, Leeor Kronik
Aug 21, 2019·Journal of Chemical Theory and Computation·Maria Hellgren, Tim Gould

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