Concurrent Learning Scheme for Crystal Structure Prediction

Crystal structure prediction (CSP) and machine learning potential (MLP) are two fundamental methods for modern computational material discovery. While the former aims at efficient sampling of the potential energy surface (PES) for discovering new materials, the latter focuses on reproducing the PES to accelerate various atomic simulation tasks. In this work, we combine the two methods within a concurrent learning framework in an effort to generate efficient MLP models for accelerating CSP. The proposed scheme explores the PES through the swarm-intelligence calypso method, labels the most representative structures with quantum mechanical calculations, and learns the PES through a deep potential (DP) model. The process proceeds in an iterative, computationally efficient, and automated manner, leading to the collection of a most compact reference training set from which the resulting DP model is proven particularly suitable for accelerating calypso structure prediction. The scheme has been systematically benchmarked on binary magnesium-aluminium (Mg-Al) alloys and ternary lithium-lanthanum-hydrogen (Li-La-H) superhydrides, demonstrating its efficiency and reliability in DP model construction and calypso structure prediction. The proposed scheme represents a promising routine to perform the structure prediction of large or multicomponent systems.