Do the main claims made in the abstract and introduction accurately reflect the paper's Did you state the full set of assumptions of all theoretical results? Did you include complete proofs of all theoretical results? If you ran experiments... (a) Did you include the code, data, and instructions needed to reproduce the main experimental results (either in the supplemental material or as a URL)? [Y es] (b) Did you specify all the training details (e.g., data splits, hyperparameters, how they Did you report error bars (e.g., with respect to the random seed after running experiments multiple times)? Did you include the total amount of compute and the type of resources used (e.g., type Did you include any new assets either in the supplemental material or as a URL? [Y es] Did you discuss whether and how consent was obtained from people whose data you're If you used crowdsourcing or conducted research with human subjects... (a) Did you include the full text of instructions given to participants and screenshots, if applicable? [N/A] Neither crowdsourcing nor research on human subjects was However, compared to the inter-atomic distances in Euclidean space, for which specific knowledge e.g. about bond lengths or interaction length scales exits, this is not the case for the rather abstract space of SPHCs. Different parameters are used for the feature and SPHC updates, respectively.

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.