A reciprocal-space formulation of surface hopping

Alex Krotz, Roel Tempelaar*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

Surface hopping has seen great success in describing molecular phenomena where electronic excitations tend to be localized, but its application to materials with band-like electronic properties has remained limited. Here, we derive a formulation of fewest-switches surface hopping where both the quantum and classical equations of motion are solved entirely in terms of reciprocal-space coordinates. The resulting method is directly compatible with band structure calculations and allows for the efficient description of band-like phenomena by means of a truncation of the Brillouin zone. Using the Holstein and Peierls models as examples, we demonstrate the formal equivalence between real-space and reciprocal-space surface hopping and assess their accuracy against mean-field mixed quantum-classical dynamics and numerically exact results. Having very similar equations of motion, reciprocal-space surface hopping can be straightforwardly incorporated in existing (real-space) surface hopping implementations.

Original languageEnglish (US)
Article number024105
JournalJournal of Chemical Physics
Volume156
Issue number2
DOIs
StatePublished - Jan 14 2022

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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