Current-induced forces for nonadiabatic molecular dynamics

TL;DR

This paper derives a comprehensive first principles expression for current-induced forces in non-equilibrium molecular systems, enabling more accurate nonadiabatic molecular dynamics simulations with quantum effects.

Contribution

It introduces a general, first principles formulation for current-induced forces applicable to arbitrary intra-molecular interactions and electron-nuclei couplings, advancing nonadiabatic molecular dynamics.

Findings

Provides a controlled way to include quantum nuclear effects.

Accounts for non-Markovian electronic friction.

Connects with previous theoretical studies.

Abstract

We present general first principles derivation of expression for current-induced forces. The expression is applicable in non-equilibrium molecular systems with arbitrary intra-molecular interactions and for any electron-nuclei coupling. It provides a controlled consistent way to account for quantum effects of nuclear motion, accounts for electronic non-Markov character of the friction tensor, and opens way to treatments beyond strictly adiabatic approximation. We show connection of the expression with previous studies, and discuss effective ways to evaluate the friction tensor.