A Reciprocal-Space Formulation of Surface Hopping

Alex Krotz; Roel Tempelaar

doi:10.1063/5.0076070

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arXiv · 2110.13777

A Reciprocal-Space Formulation of Surface Hopping

Alex Krotz·Roel Tempelaar

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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.

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Alex Krotz, Roel Tempelaar. 2021-10-26. A Reciprocal-Space Formulation of Surface Hopping. https://doi.org/10.1063/5.0076070

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