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.
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14 January 2022
Research Article|
January 10 2022
A reciprocal-space formulation of surface hopping
Special Collection:
2021 JCP Emerging Investigators Special Collection
Alex Krotz
;
Alex Krotz
Department of Chemistry, Northwestern University
, 2145 Sheridan Road, Evanston, Illinois 60208, USA
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Roel Tempelaar
Roel Tempelaar
a)
Department of Chemistry, Northwestern University
, 2145 Sheridan Road, Evanston, Illinois 60208, USA
a)Author to whom correspondence should be addressed: roel.tempelaar@northwestern.edu
Search for other works by this author on:
a)Author to whom correspondence should be addressed: roel.tempelaar@northwestern.edu
Note: This paper is part of the 2021 JCP Emerging Investigators Special Collection.
J. Chem. Phys. 156, 024105 (2022)
Article history
Received:
October 20 2021
Accepted:
December 22 2021
Citation
Alex Krotz, Roel Tempelaar; A reciprocal-space formulation of surface hopping. J. Chem. Phys. 14 January 2022; 156 (2): 024105. https://doi.org/10.1063/5.0076070
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