Low-cost orbital-based linear-scaling \emph{ab initio} molecular dynamics for weakly-interacting systems

TL;DR

This paper introduces a low-cost, linear-scaling ab initio molecular dynamics method tailored for weakly-interacting systems, enabling efficient and large-scale simulations by maintaining localized orbitals without density matrix optimization.

Contribution

The authors develop a robust orbital-only molecular dynamics approach within linear-scaling DFT that simplifies computations for weakly-interacting systems, avoiding density matrix optimization.

Findings

Efficient orbital-only MD method with low computational overhead.

Linear-scaling complexity enables large-scale simulations.

Successful application to liquid water demonstrates practicality.

Abstract

Within the framework of linear-scaling Kohn-Sham density functional theory, a robust method for maintaining compact localized orbitals close to the ground state is coupled with nuclear dynamics. This allows to obviate the commonly employed optimization of the one-electron density matrix and thus create an efficient orbital-only molecular dynamics method for weakly-interacting systems. An application to liquid water demonstrates that the low computational overhead of the method makes it well-suited for routine simulations whereas its linear-scaling complexity allows to extend first-principle dynamical studies of molecular systems to previously inaccessible length scales.