Accelerating materials discovery with Bayesian optimization and graph deep learning

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 (P6(3)=mmc) and ReWB (Pca2(1)) 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.

Automated summary

The utilization of Bayesian optimization with symmetry constraints and a graph deep learning energy model allows for DFT-free relaxations of crystal structures, significantly improving the accuracy of ML-predicted properties and leading to the discovery and synthesis of novel ultra-incompressible hard crystals with exceptional properties.