Transferable Kinetic Monte Carlo Models with Thousands of Reactions Learned from Molecular Dynamics Simulations.

Abstract

Molecular dynamics (MD) simulation of complex chemistry typically involves thousands of atoms propagating over millions of time steps, generating a wealth of data. Traditionally these data are used to calculate some aggregate properties of the system and then discarded, but we propose that these data can be reused to study related chemical systems. Using approximate chemical kinetic models and methods from statistical learning, we study hydrocarbon chemistries under extreme thermodynamic conditions. We discover that a single MD simulation can contain sufficient information about reactions and rates to predict the dynamics of related yet different chemical systems using kinetic Monte Carlo (KMC) simulation. Our learned KMC models identify thousands of reactions and run 4 orders of magnitude faster than MD. The transferability of these models suggests that we can viably reuse data from existing MD simulations to accelerate future simulation studies and reduce the number of new MD simulations required.