Machine-learnt potential highlights melting and freezing of aluminum nanoparticles

Abstract

We investigated the complete thermodynamic cycle of aluminum nanoparticles through classical molecular dynamics simulations, spanning a wide size range from 200 atoms to 11 000 atoms. The aluminum–aluminum interactions are modeled using a newly developed Bayesian Force Field (BFF) from the FLARE suite, a cutting-edge tool in our field. We discuss the database requirements to include melted nanodroplets to avoid unphysical behavior at the phase transition. Our study provides a comprehensive understanding of structural stability up to sizes as large as 3 × 105 atoms. The developed Al-BFF predicts an icosahedral stability range up to 2000 atoms, ∼2 nm, followed by a region of stability for decahedra, up to 25 000 atoms. Beyond this size, the expected structure favors face-centered cubic shapes. At a fixed heating/cooling rate of 100 K/ns, we consistently observe a hysteresis loop, where the melting temperatures are higher than those associated with solidification. The annealing of a liquid droplet further stabilizes icosahedral structures, extending their stability range to 5000 atoms. Using a hierarchical k-means clustering, we find no evidence of surface melting but observe some mild indication of surface freezing. In any event, the liquid droplet’s surface shows local structural order at all sizes.