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.
Search DOE PAGES for author "Kasper, Joseph M."
Search DOE PAGES for ORCID "000000023840484X"
Search orcid.org for ORCID "000000023840484X"
Search DOE PAGES for author "Sun, Shichao"
Search DOE PAGES for ORCID "0000000276803972"
Search orcid.org for ORCID "0000000276803972"
Search DOE PAGES for author "Li, Xiaosong"
Search DOE PAGES for ORCID "0000000173416240"
Search orcid.org for ORCID "0000000173416240"
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.