Real time propagation of the exact two component time-dependent density functional theory

Goings, Joshua J.; Kasper, Joseph M.; Egidi, Franco; Sun, Shichao; Li, Xiaosong

doi:10.1063/1.4962422

Title: Real time propagation of the exact two component time-dependent density functional theory

Journal Article · Tue Sep 13 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4962422· OSTI ID:1467884

Goings, Joshua J. ^[1];

^[1]; Egidi, Franco ^[1];

^[1];

^[1]

Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry

We report the development of a real time propagation method for solving the time-dependent relativistic exact two-component density functional theory equations (RT-X2C-TDDFT). The method is fundamentally non-perturbative and may be employed to study nonlinear responses for heavy elements which require a relativistic Hamiltonian. Here, we apply the method to several group 12 atoms as well as heavy-element hydrides, comparing with the extensive theoretical and experimental studies on this system, which demonstrates the correctness of our approach. Because the exact two-component Hamiltonian contains spin-orbit operators, the method is able to describe the non-zero transition moment of otherwise spin-forbidden processes in non-relativistic theory. Furthermore, the two-component approach is more cost effective than the full four-component approach, with similar accuracy. The RT-X2C-TDDFT will be useful in future studies of systems containing heavy elements interacting with strong external fields.

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Research Organization:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: SC0006863

OSTI ID:: 1467884

Alternate ID(s):: OSTI ID: 1324365

Journal Information:: Journal of Chemical Physics, Vol. 145, Issue 10; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 65 works

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