Review
Open access
Molecular modelling of high-entropy alloys: from quantum to atomistic, and machine learning
M. Pellegrino
Mokhtar Ganjali Koli
Fabiano Tarulli
Joseph E. Arnold
D. Mitrică
L. Bergamasco
Gonzalo García Fuentes
R. Piticescu
B. Gurrutxaga-Lerma
Matteo Fasano
Abstract
High-entropy alloys (HEAs), characterized by complex multielement compositions, offer broad opportunities to tune mechanical, corrosion, thermal, wetting, and functional properties, while their vast configurational space makes molecular modelling essential. This review evaluates progress across computational thermodynamics, density functional theory, atomistic simulations, and machine learning approaches, highlighting multiscale integration, methodological advances, current challenges, validation needs, and future directions for predictive HEA modelling and materials design across industrial applications and engineering practice.