Part of Advances in Neural Information Processing Systems 35 (NeurIPS 2022) Main Conference Track
Thorben Frank, Oliver Unke, Klaus-Robert Müller
The application of machine learning methods in quantum chemistry has enabled the study of numerous chemical phenomena, which are computationally intractable with traditional ab-initio methods. However, some quantum mechanical properties of molecules and materials depend on non-local electronic effects, which are often neglected due to the difficulty of modeling them efficiently. This work proposes a modified attention mechanism adapted to the underlying physics, which allows to recover the relevant non-local effects. Namely, we introduce spherical harmonic coordinates (SPHCs) to reflect higher-order geometric information for each atom in a molecule, enabling a non-local formulation of attention in the SPHC space. Our proposed model So3krates - a self-attention based message passing neural network - uncouples geometric information from atomic features, making them independently amenable to attention mechanisms. Thereby we construct spherical filters, which extend the concept of continuous filters in Euclidean space to SPHC space and serve as foundation for a spherical self-attention mechanism. We show that in contrast to other published methods, So3krates is able to describe non-local quantum mechanical effects over arbitrary length scales. Further, we find evidence that the inclusion of higher-order geometric correlations increases data efficiency and improves generalization. So3krates matches or exceeds state-of-the-art performance on popular benchmarks, notably, requiring a significantly lower number of parameters (0.25 - 0.4x) while at the same time giving a substantial speedup (6 - 14x for training and 2 - 11x for inference) compared to other models.