Fine-tuning of universal machine-learning interatomic potentials for high-entropy alloys with application to 2D (Mo,Ta,Nb,W,V)S$_2$

Abstract

High-entropy alloy (HEA) materials and their two-dimensional counterparts (2D-HEAs) have recently attracted attention due to their tunable properties and catalytic potential, yet their chemical complexity makes direct density functional theory (DFT) calculations computationally prohibitive. The complexity also makes training of machine-learning interatomic potentials (MLIPs) challenging, but this could possibly be overcome by employing universal MLIPs as starting point. In this work, we investigate the applicability of universal MLIP models for 2D transition metal dichalcogenide HEAs and develop effective fine-tuning strategies. Training structures are systematically generated and selected, and the performance of universal and fine-tuned models are benchmarked against DFT. We find that all universal MLIPs employed in this work yield unsatisfactory mixing energies without fine-tuning. Applied to the experimentally synthesized (Mo,Ta,Nb,W,V)S$_2$ system, fine-tuned models based on enumerated structures can achieve near-DFT accuracy in predicting mixing energies while enabling Monte-Carlo simulations and random structure sampling at scales inaccessible to DFT.