Surface hopping in laser-driven molecular dynamics

T. Fiedlschuster, J. Handt, E. K.U. Gross, R. Schmidt*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

21 Scopus citations

Abstract

A theoretical justification of the empirical surface hopping method for the laser-driven molecular dynamics is given by utilizing the formalism of the exact factorization of the molecular wave function [Abedi, Phys. Rev. Lett. 105, 123002 (2010)PRLTAO0031-900710.1103/PhysRevLett.105.123002] in its quantum-classical limit. Employing an exactly solvable H2+-like model system, it is shown that the deterministic classical nuclear motion on a single time-dependent surface in this approach describes the same physics as stochastic (hopping-induced) motion on several surfaces, provided Floquet surfaces are applied. Both quantum-classical methods do describe reasonably well the exact nuclear wave-packet dynamics for extremely different dissociation scenarios. Hopping schemes using Born-Oppenheimer surfaces or instantaneous Born-Oppenheimer surfaces fail completely.

Original languageAmerican English
Article number063424
JournalPhysical Review A
Volume95
Issue number6
DOIs
StatePublished - 28 Jun 2017
Externally publishedYes

Bibliographical note

Publisher Copyright:
© 2017 American Physical Society.

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