A reciprocal-space formulation of mixed quantum–classical dynamics
- 8 June 2021
- journal article
- research article
- Published by AIP Publishing in The Journal of Chemical Physics
- Vol. 154 (22), 224101
- https://doi.org/10.1063/5.0053177
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.This publication has 52 references indexed in Scilit:
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