Exploring non-adiabatic approximations to the exchange–correlation functional of TDDFT

Fuks, Johanna I.; Lacombe, Lionel; Nielsen, Søren E.  B.; Maitra, Neepa T.

doi:10.1039/c8cp03957g

Exploring non-adiabatic approximations to the exchange–correlation functional of TDDFT

Journal Article · Tue Oct 02 00:00:00 EDT 2018 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c8cp03957g· OSTI ID:1612279

^[1]; Lacombe, Lionel ^[2]; Nielsen, Søren E. B. ^[3]; ^[2]

Univ. of Buenos Aires (Argentina); DOE/OSTI
City Univ. of New York (CUNY), NY (United States)
Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science, Hamburg (Germany)

A decomposition of the exact exchange–correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non-adiabatic approximations. The components are expressed in terms of the exchange–correlation hole and the difference between the one-body density matrix of the interacting and Kohn–Sham systems, which must be approximated in terms of quantities accessible from the Kohn–Sham evolution. We explore several preliminary approximations, evaluate their fulfillment of known exact conditions, and test their performance on simple model systems for which available exact solutions indicate the significance of going beyond the adiabatic approximation.

View Accepted Manuscript (DOE)

Research Organization:: City University of New York (CUNY), NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0015344

OSTI ID:: 1612279

Alternate ID(s):: OSTI ID: 1477207

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 41 Vol. 20; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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