Classical nuclear motion coupled to electronic non-adiabatic transitions

TL;DR

This paper introduces a new mixed quantum-classical method for simulating non-adiabatic processes, derived from the exact electron-nuclear wave function factorization, and validates it with numerical tests on a charge transfer model.

Contribution

It presents a novel zero-th order approximation scheme for coupled electron-nuclear dynamics based on wave function factorization, with validation through numerical experiments.

Findings

The method accurately captures non-adiabatic charge transfer dynamics.

Numerical tests validate the effectiveness of the approximation.

The approach provides a new framework for mixed quantum-classical simulations.

Abstract

We present a detailed derivation and numerical tests of a new mixed quantum-classical scheme to deal with non-adiabatic processes. The method is presented as the zero-th order approximation to the exact coupled dynamics of electrons and nuclei offered by the factorization of the electron-nuclear wave function [A. Abedi, N. T. Maitra and E. K. U. Gross, Phys. Rev. Lett., 105 (2010)]. Numerical results are presented for a model system for non-adiabatic charge transfer in order to test the performance of the method and to validate the underlying approximations.