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

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.
Authors:
 [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ; ORCiD logo [1]
  1. Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
SC0006863
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 10; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org:
USDOE; National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1467884
Alternate Identifier(s):
OSTI ID: 1324365

Goings, Joshua J., Kasper, Joseph M., Egidi, Franco, Sun, Shichao, and Li, Xiaosong. Real time propagation of the exact two component time-dependent density functional theory. United States: N. p., Web. doi:10.1063/1.4962422.
Goings, Joshua J., Kasper, Joseph M., Egidi, Franco, Sun, Shichao, & Li, Xiaosong. Real time propagation of the exact two component time-dependent density functional theory. United States. doi:10.1063/1.4962422.
Goings, Joshua J., Kasper, Joseph M., Egidi, Franco, Sun, Shichao, and Li, Xiaosong. 2016. "Real time propagation of the exact two component time-dependent density functional theory". United States. doi:10.1063/1.4962422. https://www.osti.gov/servlets/purl/1467884.
@article{osti_1467884,
title = {Real time propagation of the exact two component time-dependent density functional theory},
author = {Goings, Joshua J. and Kasper, Joseph M. and Egidi, Franco and Sun, Shichao and Li, Xiaosong},
abstractNote = {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.},
doi = {10.1063/1.4962422},
journal = {Journal of Chemical Physics},
number = 10,
volume = 145,
place = {United States},
year = {2016},
month = {9}
}