Evolutionary computing and machine learning for the discovering of low-energy defect configurations

Abstract: Density functional theory (DFT) has become a standard tool for the study of point defects in materials. However, finding the most stable defective structures remains a very challenging task as it involves the solution of a multimodal optimization problem with a high-dimensional objective function. Hitherto, the approaches most commonly used to tackle this problem have been mostly empirical, heuristic and/or based on domain knowledge. In this contribution, we describe an approach for exploring the potential energy surface based on the covariance matrix adaption evolution strategy (CMA-ES) and supervised and unsupervised machine learning models. We show how the original CMA-ES can be modified to suit the specific problem of DFT studies of point defects in the dilute limit. The resulting algorithm depends only on a limited set of physically interpretable hyperparameters. The approach offers a robust and systematic way for finding low-energy configurations of point defects in solids. We demonstrate the applicability and moderate computational cost on the intrinsic defects in silicon. We also apply the methodology to the neutral oxygen vacancy oxygen vacancy in TiO$_2$ anatase and reproduce the known defect structures. Furthermore, a new defect structure, stable at the level of hybrid density functional theory and characterized by a delocalized electronic structure, is found for this system.