## Abstract

We derive a formulation of mixed quantum-classical dynamics for modeling electronic carriers interacting with phonons in reciprocal space. For dispersionless phonons, we start by expressing the real-space classical coordinates in terms of complex variables. Taking these variables as a Fourier series then yields the reciprocal-space coordinates. Evaluating the electron-phonon interaction term through Ehrenfest's theorem, we arrive at a reciprocal-space formalism that is equivalent to mean-field mixed quantum-classical dynamics in real space. This equivalence is numerically verified for the Holstein and Peierls models, for which we find the reciprocal-space Hellmann-Feynman forces to involve momentum-derivative contributions in addition to the position-derivative terms commonly seen in real space. To illustrate the advantage of the reciprocal-space formulation, we present a proof of concept for the inexpensive modeling of low-momentum carriers interacting with phonons using a truncated reciprocal-space basis, which is not possible within a real-space formulation.

Original language | English (US) |
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Article number | 224101 |

Journal | Journal of Chemical Physics |

Volume | 154 |

Issue number | 22 |

DOIs | |

State | Published - Jun 14 2021 |

## ASJC Scopus subject areas

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