Driving force of atomic ordering in Fe-Pt alloys, investigated by density functional theory and machine-learning interatomic potentials Monte Carlo simulations.

Abstract

We report the mechanisms of atomic ordering in Fe-Pt bimetallic alloys using density functional theory (DFT) and machine-learning interatomic potential Monte Carlo (MLIP-MC) simulations. We clarified that the formation enthalpy of the ordered phase was significantly enhanced by spin polarization compared to that of the disordered phase. Analysis of the density of states indicated that coherence in local potentials in the ordered phase brings energy gain over the disordered phase, when spin is considered. MLIP-MC simulations were performed to investigate the phase transition of atomic ordering at finite temperatures. The model trained using the DFT dataset with spin polarization exhibited quantitatively good agreement with previous experiments and thermodynamic calculations across a wide range of Pt compositions. In contrast, the model without spin significantly underestimated the transition temperature. Through this study, we clarified that spin polarization is essential for accurately accounting for the ordered phase in Fe-Pt bimetallic alloys, even above the Curie temperature, possibly because of the remaining short-range spin order.