Reduced computational cost of polarizable force fields by a modification of the always stable predictor-corrector

Abstract

Classical polarizable force fields effectively incorporate the dynamic response of the electronic charge distributions into molecular dynamics simulations, but they do so at a significant increase in computational cost compared to simpler models. Here, we demonstrate how one can improve the stability of a polarizable force field molecular dynamics simulation or accelerate the evaluation of self-consistent polarization via a simple extension of the predictor in the always stable predictor-corrector method. Specifically, increasing the number of prior steps used in the predictor from 6 to 16 reduces the energy drift by an order of magnitude. Alternatively, for a given level of energy drift, the induced dipoles can be obtained ∼20% faster due to the reduced number of self-consistent field iterations required to maintain energetic stability. The extended-history predictor is straightforward to implement and involves minimal computational overhead.