Graph attention neural networks for mapping materials and molecules beyond short-range interatomic correlations

Abstract

Abstract Bringing advances in machine learning to chemical science is leading to a revolutionary change in the way of accelerating materials discovery and atomic-scale simulations. Currently, most successful machine learning schemes can be largely traced to the use of localized atomic environments in the structural representation of materials and molecules. However, this may undermine the reliability of machine learning models for mapping complex systems and describing long-range physical effects because of the lack of non-local correlations between atoms. To overcome such limitations, here we report a graph attention neural network as a unified framework to map materials and molecules into a generalizable and interpretable representation that combines local and non-local information of atomic environments from multiple scales. As an exemplary study, our model is applied to predict the electronic structure properties of metal-organic frameworks (MOFs) which have notable diversity in compositions and structures. The results show that our model achieves the state-of-the-art performance. The clustering analysis further demonstrates that our model enables high-level identification of MOFs with spatial and chemical resolution, which would facilitate the rational design of promising reticular materials. Furthermore, the application of our model in predicting the heat capacity of complex nanoporous materials, a critical property in a carbon capture process, showcases its versatility and accuracy in handling diverse physical properties beyond electronic structures.