Data efficient machine learning potentials for modeling catalytic reactivity via active learning and enhanced sampling

Abstract

Simulating catalytic reactivity under operative conditions poses a significant challenge due to the dynamic nature of the catalysts and the high computational cost of electronic structure calculations. Machine learning potentials offer a promising avenue to simulate dynamics at a fraction of the cost, but they require datasets containing all relevant configurations, particularly reactive ones. Here, we present a scheme to construct reactive potentials in a data-efficient manner. This is achieved by combining enhanced sampling methods first with Gaussian processes to discover transition paths and then with graph neural networks to obtain a uniformly accurate description. The necessary configurations are extracted via a Data-Efficient Active Learning (DEAL) procedure based on local environment uncertainty. We validated our approach by studying several reactions related to the decomposition of ammonia on iron-cobalt alloy catalysts. Our scheme proved to be efficient, requiring only ~1000 DFT calculations per reaction, and robust, sampling reactive configurations from the different accessible pathways. Using this potential, we calculated free energy profiles and characterized reaction mechanisms, showing the ability to provide microscopic insights into complex processes under dynamic conditions.