Probabilistic prediction of material stability: integrating convex hulls into Bayesian active learning


Active learning is a valuable tool for efficiently exploring complex spaces, finding a variety of uses in materials science. However, the determination of convex hulls for phase diagrams does not neatly fit into traditional active learning approaches due to their global nature. Specifically, the thermodynamic stability of a material is not a function of the energies associated with a single composition, including information from all other competing compositions. Here we present Convex Hull-aware Active Learning (CAL), a novel Bayesian algorithm that chooses experiments to minimize the uncertainty in the convex hull. CAL prioritizes compositions that are close to or on the hull, leaving significant uncertainty in other compositions that are quickly determined to be irrelevant to the convex hull. The convex hull can thus be predicted with significantly fewer observations than approaches that focus solely on energy. Intrinsic to the Bayesian approach is uncertainty quantification in both the convex hull and all subsequent predictions (e.g., stability and chemical potential). By providing increased search efficiency and uncertainty quantification, CAL can be readily incorporated into the emerging paradigm of uncertainty-based workflows for thermodynamic prediction.

arXiv preprint