Can MACE Potentials Accurately Describe Magnetism and Phase Stability in Fe-Ni Alloys? A Systematic Benchmark

Abstract

We present a systematic benchmark of MACE potentials for iron-nickel alloys, focusing on structural, elastic, magnetic, and finite-temperature properties relevant to phase stability. The reference dataset comprises spin-polarized PBE density functional theory (DFT) calculations for chemically disordered special quasirandom structures (SQS), spanning compositions, bcc and fcc crystal structures, and volumetric and shear deformations. A system-specific MACE-sqs model trained on this dataset achieves validation errors of 2.0 meV/atom for energies and 24.3 meV/Angstrom for forces. Compared with several MACE foundation models, including models trained with Hubbard U corrections, MACE-sqs gives the most consistent agreement with DFT and experiment for equations of state, equilibrium volumes, elastic constants, and thermal expansion trends in bcc and fcc Fe-Ni alloys. For the bcc-to-hcp transition, MACE-sqs predicts a pure-Fe transition pressure closer to experiment than the tested foundation models, but all models predict an incorrect increase of transition pressure with Ni content. This failure indicates that high-pressure magnetic collapse and composition-dependent magnetoelastic effects are not yet fully captured. Overall, targeted SQS-based training substantially improves the accuracy of MACE potentials for Fe-Ni alloys, while phase stability under magnetic collapse remains a key limitation for future model development.