SE(3)-equivariant prediction of molecular wavefunctions and electronic densities

Oliver Thorsten Unke, Mihail Bogojeski, Michael Gastegger, Mario Geiger, Tess Smidt, Klaus Robert Muller

Keywords: Deep learning, quantum chemistry, steerable networks, message passing networks

TL;DR: We introduce a deep learning model that is capable of predicting molecular wavefunctions via the Hamiltonian matrix to an unprecedented accuracy.

Abstract: Machine learning has enabled the prediction of quantum chemical properties with high accuracy and efficiency, allowing to bypass computationally costly ab initio calculations. Instead of training on a fixed set of properties, more recent approaches attempt to learn the electronic wavefunction (or density) as a central quantity of atomistic systems, from which all other observables can be derived. This is complicated by the fact that wavefunctions transform non-trivially under molecular rotations, which makes them a challenging prediction target. To solve this issue, we introduce general SE(3)-equivariant operations and building blocks for constructing deep learning architectures for geometric point cloud data and apply them to reconstruct wavefunctions of atomistic systems with unprecedented accuracy. Our model achieves speedups of over three orders of magnitude compared to ab initio methods and reduces prediction errors by up to two orders of magnitude compared to the previous state-of-the-art. This accuracy makes it possible to derive properties such as energies and forces directly from the wavefunction in an end-to-end manner. We demonstrate the potential of our approach in a transfer learning application, where a model trained on low accuracy reference wavefunctions implicitly learns to correct for electronic many-body interactions from observables computed at a higher level of theory. Such machine-learned wavefunction surrogates pave the way towards novel semi-empirical methods, offering resolution at an electronic level while drastically decreasing computational cost. Additionally, the predicted wavefunctions can serve as initial guess in conventional ab initio methods, decreasing the number of iterations required to arrive at a converged solution, thus leading to significant speedups without any loss of accuracy or robustness. While we focus on physics applications in this contribution, the proposed equivariant framework for deep learning on point clouds is promising also beyond, say, in computer vision or graphics.

Code Of Conduct: I certify that all co-authors of this work have read and commit to adhering to the NeurIPS Statement on Ethics, Fairness, Inclusivity, and Code of Conduct.