Discovering new photovoltaics using optimal transport theory

Searching by chemical and structural analogy is one of the most commonly used and successful approaches to materials discovery. However, formulating this task for algorithmic implementation raises the question of how we define similar materials. Methods have been proposed for searching materials space using vectors based on chemical composition and functional fragments in the material. Descriptors for structural similarity have also been proposed. However, the question of how to incorporate and balance structural and compositional similarity measures in a single metric remains open. Here, we adapt methods developed for calculating distances between undirected graphs and apply them to crystalline materials similarity. The Fused Gromov-Wasserstein (FGW) metric uses optimal transport theory to map between two graphs considering a balance of the graph structure and the information present at the nodes of the graph (atoms in crystals). We apply the method to explore new photovoltaic materials. We demonstrate that FGW is competitive with embeddings from an equivariant graph neural network, trained on >10⁶ materials, despite minimal training. We then apply FGW to a discovery campaign to identify materials from the Materials Project database that have not previously been explored as photovoltaics, but have similarities to known high-efficiency materials. After validating predictions with hybrid density functional theory, we identify seven previously unexplored high-efficiency photovoltaic absorber candidates, including Cs₅Sb₈, which is found to have a predicted SLME of >30% and to be thermodynamically stable. The FGW approach demonstrates the power of strong inductive bias for developing metrics for materials exploration with minimal training data.