Iterative learning scheme for crystal structure prediction with anharmonic lattice dynamics

Abstract

First-principles based crystal structure prediction (CSP) methods have revealed an essential tool for the discovery of new materials. However, in solids close to displacive phase transitions, which are common in ferroelectrics, thermoelectrics, charge-density wave systems, or superconducting hydrides, the ionic contribution to the free energy and lattice anharmonicity become essential, limiting the capacity of CSP techniques to determine the thermodynamical stability of competing phases. While variational methods like the stochastic self-consistent harmonic approximation (SSCHA) accurately account for anharmonic lattice dynamics \emph{ab initio}, their high computational cost makes them impractical for CSP. Machine-learning interatomic potentials offer accelerated sampling of the energy landscape compared to purely first-principles approaches, but their reliance on extensive training data and limited generalization restricts practical applications. Here, we propose an iterative learning framework combining evolutionary algorithms, atomic foundation models, and SSCHA to enable CSP with anharmonic lattice dynamics. Foundation models enable robust relaxations of random structures, drastically reducing required training data. Applied to the highly anharmonic H${}_3$S system, our framework achieves good agreement with the benchmarks based on density functional theory, accurately predicting phase stability and vibrational properties from 50 to 200 GPa. Importantly, we find that the statistical averaging in the SSCHA reduces the error in the free energy evaluation, avoiding the need for extremely high accuracy of machine-learning potentials. This approach bridges the gap between data efficiency and predictive power, establishing a practical pathway for CSP with anharmonic lattice dynamics.

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