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  Time-dependent density functional theory beyond Kohn–Sham Slater determinants

Fuks, J. I., Nielsen, S. E. B., Ruggenthaler, M., & Maitra, N. T. (2016). Time-dependent density functional theory beyond Kohn–Sham Slater determinants. Physical Chemistry Chemical Physics, 18(31), 20976-20985. doi:10.1039/C6CP00722H.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-2083-8 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-2084-6
Genre: Journal Article

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1603.01176v2.pdf (Preprint), 782KB
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© J. I. Fuks et al.

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http://dx.doi.org/10.1039/C6CP00722H (Publisher version)
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https://arxiv.org/abs/1603.01176 (Preprint)
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 Creators:
Fuks, Johanna I.1, Author
Nielsen, Søren Ersbak Bang2, 3, 4, Author              
Ruggenthaler, Michael2, 3, 4, Author              
Maitra, Neepa T.1, Author
Affiliations:
1Department of Physics and Astronomy, Hunter College and the Graduate Center of the City University of New York, 695 Park Avenue, New York, USA, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science & Department of Physics, Luruper Chaussee 149, 22761 Hamburg, Germany, ou_persistent22              
4Institut für Theoretische Physik, Universität Innsbruck, Technikerstraße 21A, A-6020 Innsbruck, Austria, ou_persistent22              

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Free keywords: Chemical Physics; Density Functional Theory
 Abstract: When running time-dependent density functional theory (TDDFT) calculations for real-time simulations of non-equilibrium dynamics, the user has a choice of initial Kohn–Sham state, and typically a Slater determinant is used. We explore the impact of this choice on the exchange–correlation potential when the physical system begins in a 50 : 50 superposition of the ground and first-excited state of the system. We investigate the possibility of judiciously choosing a Kohn–Sham initial state that minimizes errors when adiabatic functionals are used. We find that if the Kohn–Sham state is chosen to have a configuration matching the one that dominates the interacting state, this can be achieved for a finite time duration for some but not all such choices. When the Kohn–Sham system does not begin in a Slater determinant, we further argue that the conventional splitting of the exchange–correlation potential into exchange and correlation parts has limited value, and instead propose a decomposition into a “single-particle” contribution that we denote vSxc, and a remainder. The single-particle contribution can be readily computed as an explicit orbital-functional, reduces to exchange in the Slater determinant case, and offers an alternative to the adiabatic approximation as a starting point for TDDFT approximations.

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Language(s): eng - English
 Dates: 2016-02-012016-03-072016-03-072016-08-21
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1039/C6CP00722H
arXiv: 1603.01176
 Degree: -

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Title: Physical Chemistry Chemical Physics
  Abbreviation : Phys. Chem. Chem. Phys.
Source Genre: Journal
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Publ. Info: Cambridge, England : Royal Society of Chemistry
Pages: - Volume / Issue: 18 (31) Sequence Number: - Start / End Page: 20976 - 20985 Identifier: ISSN: 1463-9076
CoNE: /journals/resource/954925272413_1