Equivariant Neural Networks Utilizing Molecular Clusters for Accurate Molecular Crystal Binding Energy Predictions

Equivariant neural networks have emerged as prominent models in advancing the construction of interatomic potentials due to their remarkable data efficiency and generalization capabilities for out-of-distribution data. Here, we expand the utility of these networks to the prediction of crystal structures consisting of organic molecules. Traditional methods for computing crystal structure properties, such as plane-wave quantum chemical methods based on density functional theory (DFT), are prohibitively resource-intensive, often necessitating compromises in accuracy and the choice of exchange-correlation functional. We present an approach that leverages the efficiency, and transferability of equivariant neural networks, specifically Allegro, to predict molecular crystal structure energies at a reduced computational cost. Our neural network is trained on molecular clusters using a highly accurate Gaussian-type orbital (GTO)-based method as the target level of theory, eliminating the need for costly periodic DFT calculations, while providing access to all families of exchange-corelation functionals and post-Hartree Fock methods. The trained model exhibits remarkable accuracy in predicting binding energies, aligning closely with those computed by plane-wave based DFT methods, thus representing significant cost reductions. Furthermore, the Allegro network was seamlessly integrated with the USPEX framework, accelerating the discovery of low-energy crystal structures during crystal structure prediction.