Transforming the Accuracy and Numerical Stability of ReaxFF Reactive Force Fields.

Molecular dynamics (MD) simulations provide an important link between theories and experiments. While ab initio methods can be prohibitively costly, the ReaxFF force field has facilitated in silico studies of chemical reactivity in complex, condensed-phase systems. However, the relatively poor energy conservation in ReaxFF MD has either limited the applicability to short time scales, in cases where energy propagation is important, or has required a continuous coupling of the system to a heat bath. In this study, we reveal the root cause of the unsatisfactory energy conservation, and offer a straightforward solution. The new scheme results in orders of magnitude improvement in energy conservation, numerical stability, and accuracy of ReaxFF force fields, compared to the previous state-of-the-art, at no additional cost. We anticipate that these improvements will open new avenues of research for more accurate reactive simulations in complex systems on long time scales.