Building atomistic models of heterointerfaces with optimal transport

Abstract

Heterogeneous interfaces underpin technologies from microelectronics to energy conversion and storage, but their configurational complexity precludes exhaustive first-principles screening of interface registries. Although data-driven approaches can alleviate this burden, they remain limited by sparse interface datasets. Here, we introduce an energy-independent workflow that represents coherent interfaces as attributed graphs, quantifies their similarity to parent bulk environments using the fused Gromov-Wasserstein (FGW) distance, and couples this metric with Bayesian optimization over the in-plane registry space. We assess the approach for KI/NaCl, GaP/GaAs and GaN/$\mathrm{Al_{2}O_{3}}$ interfaces spanning ionic, covalent and mixed-bonding regimes, using hierarchical validation with MACE and density functional theory (DFT). Comparison with single-point energy landscapes shows that the FGW distance captures registry-dependent periodicity, while interfaces exhibit deviations between structural and energetic extrema, reflecting additional chemistry-specific contributions. Furthermore, FGW distances show an overall association with relaxed energies. Under limited screening budgets, FGW-guided registry selection consistently outperforms random search and is more robust across interface systems than selection guided by pretrained MACE energies. The workflow converts the qualitative notion of bulk-like continuity into a quantitative prescreening criterion, enabling efficient registry exploration and providing physically informed candidate structures for materials discovery workflows.