Exact non-adiabatic coupling vectors for the time-dependent density functional based tight-binding method

Autor:	Thomas A. Niehaus
Rok vydání:	2023
Předmět:	General Physics and Astronomy Physical and Theoretical Chemistry
Zdroj:	The Journal of Chemical Physics. 158:054103
ISSN:	1089-7690 0021-9606
Popis:	We report on non-adiabatic coupling vectors between electronic excited states for the time-dependent-density functional theory based tight-binding (TD-DFTB) method. The implementation includes orbital relaxation effects that have been previously neglected and covers also the case of range-separated exchange-correlation functionals. Benchmark calculations with respect to first principles TD-DFT highlight the large dependence of non-adiabatic couplings on the functional. Closer investigations of the topology around a conical intersection between excited states show that TD-DFTB delivers near-exact values of the Berry phase, which paves the way for consistent non-adiabatic molecular dynamics simulations for large systems.
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_________::9c5a4777487f94e401a5423cbaf8138a https://doi.org/10.1063/5.0136838 Zobrazit plný text záznamu