Surface hopping in laser-driven molecular dynamics

T. Fiedlschuster, J. Handt, E. K. U. Gross, and R. Schmidt
Phys. Rev. A 95, 063424 – Published 28 June 2017
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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 et al., Phys. Rev. Lett. 105, 123002 (2010)] 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.

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  • Received 23 August 2016
  • Revised 7 June 2017

DOI:https://doi.org/10.1103/PhysRevA.95.063424

©2017 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

T. Fiedlschuster1,2, J. Handt1, E. K. U. Gross2, and R. Schmidt1,*

  • 1Institut für Theoretische Physik, Technische Universität Dresden, D-01062 Dresden, Germany
  • 2Max-Planck-Institut für Mikrostrukturphysik, Weinberg 2, D-06120 Halle, Germany

  • *ruediger.schmidt@tu-dresden.de

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Issue

Vol. 95, Iss. 6 — June 2017

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