A Comparative Study of Machine Learning Models Predicting Energetics of Interacting Defects

Abstract

Interacting defect systems are ubiquitous in materials under realistic scenarios, yet gaining an atomic-level understanding of these systems from a computational perspective is challenging - it often demands substantial resources due to the necessity of employing supercell calculations. While machine learning techniques have shown potential in accelerating materials simulations, their application to systems involving interacting defects remains relatively rare. In this work, we present a comparative study of three different methods to predict the free energy change of systems with interacting defects. We leveraging a limited dataset from Density Functional Theory(DFT) calculations to assess the performance models using materials descriptors, graph neural networks and cluster expansion. Our findings indicate that the cluster expansion model can achieve precise energetics predictions even with this limited dataset. Furthermore, with synthetic data generate from cluster expansion model at near-DFT levels, we obtained enlarged dataset to assess the demands on data for training accurate prediction models using graph neural networks for systems featuring interacting defects. A brief discussion of the computational cost for each method is provided at the end. This research provide a preliminary evaluation of applying machine learning techniques in imperfect surface systems.