Machine learning potentials for modeling alloys across compositions (2506.12592v2)

Abstract: Materials properties depend strongly on chemical composition, i.e., the relative amounts of each chemical element. Changes in composition lead to entirely different chemical arrangements, which vary in complexity from perfectly ordered (i.e., stoichiometric compounds) to completely disordered (i.e., solid solutions). Accurately capturing this range of chemical arrangements remains a major challenge, limiting the predictive accuracy of machine learning potentials (MLPs) in materials modeling. Here, we combine information theory and machine learning to optimize the sampling of chemical motifs and design MLPs that effectively capture the behavior of metallic alloys across their entire compositional and structural landscape. The effectiveness of this approach is demonstrated by predicting the compositional dependence of various material properties - including stacking-fault energies, short-range order, heat capacities, and phase diagrams - for the AuPt and CuAu binary alloys, the ternary CrCoNi, and the TiTaVW high-entropy alloy. Extensive comparison against experimental data demonstrates the robustness of this approach in enabling materials modeling with high physical fidelity.