Fast method for quantum mechanical molecular dynamics

Abstract

As the processing power available for scientific computing grows, first-principles Born-Oppenheimer molecular dynamics simulations are becoming increasingly popular for the study of a wide range of problems in materials science, chemistry, and biology. Nevertheless, the computational cost of Born-Oppenheimer molecular dynamics still remains prohibitively large for many potential applications. Here we show how to avoid a major computational bottleneck: the self-consistent-field optimization prior to force calculations. The optimization-free quantum mechanical molecular dynamics method gives trajectories that are almost indistinguishable from an ``exact'' microcanonical Born-Oppenheimer molecular dynamics simulation even when low-prefactor linear scaling sparse matrix algebra is used. Our findings show that the computational gap between classical and quantum mechanical molecular dynamics simulations can be significantly reduced.