Automatic Process Exploration through Machine Learning Assisted Transition State Searches

We present an efficient automatic process explorer (APE) framework to overcome the reliance on human intuition to empirically establish relevant elementary processes of a given system, e.g., in prevalent kinetic Monte Carlo (kMC) simulations based on fixed process lists. Use of a fuzzy machine learning classification algorithm minimizes redundancy in the transition-state searches by driving them toward hitherto unexplored local atomic environments. APE application to island diffusion at a Pd(100) surface immediately reveals a large number of, up to now, disregarded low-barrier collective processes that lead to a significant increase in the kMC-determined island diffusivity as compared to classic surface hopping and exchange diffusion mechanisms. Published by the American Physical Society 2025