Capturing short-range order in high-entropy alloys with machine learning potentials (2401.06622v2)

Abstract: Chemical short-range order (SRO) affects the distribution of elements throughout the solid-solution phase of metallic alloys, thereby modifying the background against which microstructural evolution occurs. Investigating such chemistry-microstructure relationships requires atomistic models that act at the appropriate length scales while capturing the intricacies of chemical bonds leading to SRO. Here we consider various approaches for the construction of training data sets for machine learning potentials (MLPs) for CrCoNi and evaluate their performance in capturing SRO and its effects on materials quantities of relevance for mechanical properties, such as stacking-fault energy and phase stability. It is demonstrated that energy accuracy on test sets often does not correlate with accuracy in capturing material properties, which is fundamental in enabling large-scale atomistic simulations of metallic alloys with high physical fidelity. Based on this analysis we systematically derive design principles for the rational construction of MLPs that capture SRO in the crystal and liquid phases of alloys.