Nonadiabatic Dynamics in a Laser Field: Using Floquet Fewest Switches Surface Hopping to Calculate Electronic Populations for Slow Nuclear Velocities

Zeyu Zhou, Hsing Ta Chen, Abraham Nitzan, Joseph Eli Subotnik

Research output: Contribution to journalArticlepeer-review

Abstract

We investigate two well-known approaches for extending the fewest switches surface hopping (FSSH) algorithm to periodic time-dependent couplings. The first formalism acts as if the instantaneous adiabatic electronic states were standard adiabatic states, which just happen to evolve in time. The second formalism replaces the role of the usual adiabatic states by the time-independent adiabatic Floquet states. For a set of modified Tully model problems, the Floquet FSSH (F-FSSH) formalism gives a better estimate for both transmission and reflection probabilities than the instantaneous adiabatic FSSH (IA-FSSH) formalism, especially for slow nuclear velocities. More importantly, only F-FSSH predicts the correct final scattering momentum. Finally, in order to use Floquet theory accurately, we find that it is crucial to account for the interference between wavepackets on different Floquet states. Our results should be of interest to all those interested in laser-induced molecular dynamics.

Original languageEnglish
Pages (from-to)821-834
Number of pages14
JournalJournal of Chemical Theory and Computation
Volume16
Issue number2
DOIs
StatePublished - 11 Feb 2020
Externally publishedYes

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