Unphysical divergences in response theory

Parker, Shane M.; Roy, Saswata; Furche, Filipp

doi:10.1063/1.4963749

Unphysical divergences in response theory

Journal Article · Tue Oct 04 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4963749· OSTI ID:1464925

^[1]; Roy, Saswata ^[2]; Furche, Filipp ^[2]

Univ. of California, Irvine, CA (United States); Department of Chemistry, University of California, Irvine, 1102 Natural Sciences II, Irvine, California 92697-2025, USA
Univ. of California, Irvine, CA (United States)

Here, transition densities between excited states are key for nonlinear theoretical spectroscopy and multi-state non-adiabatic molecular dynamics (NAMD) simulations. In the framework of response theory, these transition densities are accessible from poles of the quadratic response function. It was shown recently that the thus obtained transition densities within time-dependent Hartree-Fock (TDHF) and adiabatic time-dependent density functional theory (TDDFT) exhibit unphysical divergences when the difference in excitation energy of the two states of interest matches another excitation energy.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of California, Irvine, CA (United States). Dept. of Chemistry

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0008694

OSTI ID:: 1464925

Alternate ID(s):: OSTI ID: 1328501

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 13 Vol. 145; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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