Optimization of ReaxFF parameters for the $\mathrm{Mo}-\mathrm{S}$ system using random optimization and coordinate search

Abstract

ReaxFF is a molecular dynamics method that can be considered a good approximation to quantum methods for investigating reactive molecular systems consisting of ten thousand to one hundred thousand atoms. While ReaxFF is usually a much faster alternative to quantum methods, the force field consists of nearly 100 parameters per element, which makes the force field development a high dimensional optimization problem. In addition to the high-dimensionality, non-convexity and non-continuity make it a hard problem to optimize. We use random optimization along with coordinate search strategies to optimize efficiently and sample new parameter points that yield good molecular properties close to predefined `reference values' obtained from quantum mechanical methods for the $\mathrm{Mo}-\mathrm{S}$ system. We also provide empirical error guaranties starting from any random sample of inputs. We discover new points for the $\mathrm{Mo}-\mathrm{S}$ system at adjusted error levels of $13,000$ as compared to Sengul et al. (2022) at $70,000$ levels under the same loss function, registering over $80\%$ improvement. We also extend our algorithm to an out-of-sample system, $\mathrm{W}-\mathrm{S}$, with no training data to record over $70\%$ improvement over Sengul et al. (2021).

35 pages, 15 figures, 8 tables