Year: 2023
Type: article
Abstract: When the coupled electron-nuclear dynamics are subjected to strong Floquet driving, there is a strong breakdown of the Born-Oppenheimer approximation. In this paper, we derive a Fokker-Planck equation to describe nonadiabatic molecular dynamics with electronic friction for Floquet-driven systems. We first provide a new derivation of the Floquet quantum-classical Liouville equation (QCLE) for driven electron-nuclear dynamics. We then transform the Floquet QCLE into a Fokker-Planck equation with explicit forms of frictional force and random force. We recast the electronic friction in terms of Floquet Green's functions such that we can evaluate the electronic friction explicitly. We show that the Floquet electronic friction tensor exhibits antisymmetric terms even at the equilibrium for a real-valued Hamiltonian, suggesting that there is a Lorentz-like force in Floquet-driven non-Born Oppenheimer dynamics even without any spin-orbit couplings.
Authors: Vahid Mosallanejad, Jingqi Chen, Wenjie Dou
Institution: Westlake University
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
Awards: G2728288208, G812001328
OpenAlex ID: W4380683210