Abstract: Machine learning (ML) models utilizing structure-based features provide an efficient means for accurate property predictions across diverse chemical spaces. However, obtaining equilibrium crystal structures typically requires expensive density functional theory (DFT) calculations, which limits ML-based exploration to either known crystals or a small number of hypothetical crystals. Here, we demonstrate that the application of Bayesian optimization with symmetry constraints using a graph deep learning energy model can be used to perform “DFT-free” relaxations of crystal structures. Using this approach to significantly improve the accuracy of ML-predicted formation energies and elastic moduli of hypothetical crystals, two novel ultra-incompressible hard MoWC2 (P63/mmc) and ReWB (Pca21) were identified and successfully synthesized via in situ reactive spark plasma sintering from screening 399,960 transition metal borides and carbides. This work addresses a critical bottleneck to accurate property predictions for hypothetical materials, paving the way to ML-accelerated discovery of new materials with exceptional properties.

Accelerating materials discovery with Bayesian optimization and graph deep learning
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DOI: 10.1016/j.mattod.2021.08.012