Shotgun crystal structure prediction using machine-learned formation energies

Abstract Stable or metastable crystal structures of assembled atoms can be predicted by finding the global or local minima of the energy surface within a broad space of atomic configurations. Generally, this requires repeated first-principles energy calculations, which is often impractical for large...

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Bibliographic Details
Main Authors: Liu Chang, Hiromasa Tamaki, Tomoyasu Yokoyama, Kensuke Wakasugi, Satoshi Yotsuhashi, Minoru Kusaba, Artem R. Oganov, Ryo Yoshida
Format: Article
Language:English
Published: Nature Portfolio 2024-12-01
Series:npj Computational Materials
Online Access:https://doi.org/10.1038/s41524-024-01471-8
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Summary:Abstract Stable or metastable crystal structures of assembled atoms can be predicted by finding the global or local minima of the energy surface within a broad space of atomic configurations. Generally, this requires repeated first-principles energy calculations, which is often impractical for large crystalline systems. Here, we present significant progress toward solving the crystal structure prediction problem: we performed noniterative, single-shot screening using a large library of virtually created crystal structures with a machine-learning energy predictor. This shotgun method (ShotgunCSP) has two key technical components: transfer learning for accurate energy prediction of pre-relaxed crystalline states, and two generative models based on element substitution and symmetry-restricted structure generation to produce promising and diverse crystal structures. First-principles calculations were performed only to generate the training samples and to refine a few selected pre-relaxed crystal structures. The ShotunCSP method is less computationally intensive than conventional methods and exhibits exceptional prediction accuracy, reaching 93.3% in benchmark tests with 90 different crystal structures.
ISSN:2057-3960