Extended Lagrangian Born-Oppenheimer molecular dynamics in the limit of vanishing self-consistent field optimization

TL;DR

This paper introduces an efficient first principles molecular dynamics method that eliminates the need for self-consistent field optimization, significantly reducing computational costs while maintaining accuracy.

Contribution

It presents an optimization-free extended Lagrangian Born-Oppenheimer molecular dynamics approach that requires only one diagonalization per time step, enhancing efficiency.

Findings

Reduces computational cost by eliminating SCF optimization

Maintains accuracy comparable to fully converged BO MD

Requires only one diagonalization per time step

Abstract

We present an efficient general approach to first principles molecular dynamics simulations based on extended Lagrangian Born-Oppenheimer molecular dynamics in the limit of vanishing self-consistent field optimization. The reduction of the optimization requirement reduces the computational cost to a minimum, but without causing any significant loss of accuracy or longterm energy drift. The optimization-free first principles molecular dynamics requires only one single diagonalization per time step and yields trajectories at the same level of accuracy as "exact", fully converged, Born-Oppenheimer molecular dynamics simulations. The optimization-free limit of extended Lagrangian Born-Oppenheimer molecular dynamics therefore represents an ideal starting point for a robust and efficient formulation of a new generation first principles quantum mechanical molecular dynamics simulation schemes.