000216433 001__ 216433
000216433 005__ 20180317094546.0
000216433 0247_ $$2doi$$a10.1063/1.4936864
000216433 022__ $$a0021-9606
000216433 02470 $$2ISI$$a000367194300008
000216433 037__ $$aARTICLE
000216433 245__ $$aNonadiabatic dynamics with intersystem crossings: A time-dependent density functional theory implementation
000216433 260__ $$aMelville$$bAmer Inst Physics$$c2015
000216433 269__ $$a2015
000216433 300__ $$a11
000216433 336__ $$aJournal Articles
000216433 520__ $$aIn this work, we derive a method to perform trajectory-based nonadiabatic dynamics that is able to describe both nonadiabatic transitions and intersystem crossing events (transitions between states of different spin-multiplicity) at the same level of theory, namely, time-dependent density functional theory (TDDFT). To this end, we combined our previously developed TDDFT-based trajectory surface hopping scheme with an accurate and efficient algorithm for the calculation of the spin-orbit coupling (SOC) matrix elements. More specifically, we designed two algorithms for the calculation of intersystem crossing transitions, one based on an extended Tully's surface hopping scheme including SOC and the second based on a Landau-Zener approximation applied to the spin sector of the electronic Hilbert space. This development allows for the design of an efficient on-the-fly nonadiabatic approach that can handle, on an equal footing, nonadiabatic and intersystem crossing transitions. The method is applied to the study of the photophysics of sulfur dioxide (SO2) in gas and liquid phases. (C) 2015 AIP Publishing LLC.
000216433 700__ $$aDe Carvalho, F. Franco
000216433 700__ $$aTavernelli, I.
000216433 773__ $$j143$$k22$$q224105$$tJournal Of Chemical Physics
000216433 909CO $$ooai:infoscience.tind.io:216433$$particle$$pSB
000216433 909C0 $$0252369$$pSB$$xU10077
000216433 937__ $$aEPFL-ARTICLE-216433
000216433 973__ $$aEPFL$$rREVIEWED$$sPUBLISHED
000216433 980__ $$aARTICLE