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Title: Two-component hybrid time-dependent density functional theory within the Tamm-Dancoff approximation

Abstract

We report the implementation of a two-component variant of time-dependent density functional theory (TDDFT) for hybrid functionals that accounts for spin-orbit effects within the Tamm-Dancoff approximation (TDA) for closed-shell systems. The influence of the admixture of Hartree-Fock exchange on excitation energies is investigated for several atoms and diatomic molecules by comparison to numbers for pure density functionals obtained previously [M. Kühn and F. Weigend, J. Chem. Theory Comput. 9, 5341 (2013)]. It is further related to changes upon switching to the local density approximation or using the full TDDFT formalism instead of TDA. Efficiency is demonstrated for a comparably large system, Ir(ppy){sub 3} (61 atoms, 1501 basis functions, lowest 10 excited states), which is a prototype molecule for organic light-emitting diodes, due to its “spin-forbidden” triplet-singlet transition.

Authors:
 [1];  [1]
  1. Institut für Physikalische Chemie, Karlsruher Institut für Technologie, Kaiserstraße 12, 76131 Karlsruhe (Germany)
Publication Date:
OSTI Identifier:
22416006
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 3; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; ATOMS; COMPARATIVE EVALUATIONS; DENSITY; DENSITY FUNCTIONAL METHOD; EFFICIENCY; EXCITATION; EXCITED STATES; FUNCTIONALS; HARTREE-FOCK METHOD; LIGHT EMITTING DIODES; L-S COUPLING; MOLECULES; ORBITS; TIME DEPENDENCE; TRIPLETS

Citation Formats

Kühn, Michael, Weigend, Florian, and Institut für Nanotechnologie, Karlsruher Institut für Technologie, Postfach 3640, 76021 Karlsruhe. Two-component hybrid time-dependent density functional theory within the Tamm-Dancoff approximation. United States: N. p., 2015. Web. doi:10.1063/1.4905829.
Kühn, Michael, Weigend, Florian, & Institut für Nanotechnologie, Karlsruher Institut für Technologie, Postfach 3640, 76021 Karlsruhe. Two-component hybrid time-dependent density functional theory within the Tamm-Dancoff approximation. United States. https://doi.org/10.1063/1.4905829
Kühn, Michael, Weigend, Florian, and Institut für Nanotechnologie, Karlsruher Institut für Technologie, Postfach 3640, 76021 Karlsruhe. 2015. "Two-component hybrid time-dependent density functional theory within the Tamm-Dancoff approximation". United States. https://doi.org/10.1063/1.4905829.
@article{osti_22416006,
title = {Two-component hybrid time-dependent density functional theory within the Tamm-Dancoff approximation},
author = {Kühn, Michael and Weigend, Florian and Institut für Nanotechnologie, Karlsruher Institut für Technologie, Postfach 3640, 76021 Karlsruhe},
abstractNote = {We report the implementation of a two-component variant of time-dependent density functional theory (TDDFT) for hybrid functionals that accounts for spin-orbit effects within the Tamm-Dancoff approximation (TDA) for closed-shell systems. The influence of the admixture of Hartree-Fock exchange on excitation energies is investigated for several atoms and diatomic molecules by comparison to numbers for pure density functionals obtained previously [M. Kühn and F. Weigend, J. Chem. Theory Comput. 9, 5341 (2013)]. It is further related to changes upon switching to the local density approximation or using the full TDDFT formalism instead of TDA. Efficiency is demonstrated for a comparably large system, Ir(ppy){sub 3} (61 atoms, 1501 basis functions, lowest 10 excited states), which is a prototype molecule for organic light-emitting diodes, due to its “spin-forbidden” triplet-singlet transition.},
doi = {10.1063/1.4905829},
url = {https://www.osti.gov/biblio/22416006}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 3,
volume = 142,
place = {United States},
year = {2015},
month = {1}
}