Real time propagation of the exact two component timedependent density functional theory
We report the development of a real time propagation method for solving the timedependent relativistic exact twocomponent density functional theory equations (RTX2CTDDFT). The method is fundamentally nonperturbative 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 heavyelement hydrides, comparing with the extensive theoretical and experimental studies on this system, which demonstrates the correctness of our approach. Because the exact twocomponent Hamiltonian contains spinorbit operators, the method is able to describe the nonzero transition moment of otherwise spinforbidden processes in nonrelativistic theory. Furthermore, the twocomponent approach is more cost effective than the full fourcomponent approach, with similar accuracy. The RTX2CTDDFT will be useful in future studies of systems containing heavy elements interacting with strong external fields.
 Authors:

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 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 00219606
 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 timedependent 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 timedependent 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 timedependent 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 timedependent 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 timedependent relativistic exact twocomponent density functional theory equations (RTX2CTDDFT). The method is fundamentally nonperturbative 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 heavyelement hydrides, comparing with the extensive theoretical and experimental studies on this system, which demonstrates the correctness of our approach. Because the exact twocomponent Hamiltonian contains spinorbit operators, the method is able to describe the nonzero transition moment of otherwise spinforbidden processes in nonrelativistic theory. Furthermore, the twocomponent approach is more cost effective than the full fourcomponent approach, with similar accuracy. The RTX2CTDDFT 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}
}