Learning Atomic Multipoles: Prediction of the Electrostatic Potential with Equivariant Graph Neural Networks

• Published in: Journal of chemical theory and computation 2022-03, Vol.18 (3), p.1701-1710
• Main Authors: Thürlemann, Moritz, Böselt, Lennard, Riniker, Sereina
• Format: Article
• Language: English
• Subjects: Electron density; Graph neural networks; Mathematical analysis; Molecular Mechanics; Multipoles; Neural networks; Quadrupoles
• ISSN: 1549-9618; 1549-9626
• DOI: 10.1021/acs.jctc.1c01021

The accurate description of electrostatic interactions remains a challenging problem for classical potential-energy functions. The commonly used fixed partial-charge approximation fails to reproduce the electrostatic potential at short range due to its insensitivity to conformational changes and anisotropic effects. At the same time, possibly more accurate machine-learned (ML) potentials struggle with the long-range behavior due to their inherent locality ansatz. Employing a multipole expansion offers in principle an exact treatment of the electrostatic potential such that the long-range and short-range electrostatic interactions can be treated simultaneously with high accuracy. However, such an expansion requires the calculation of the electron density using computationally expensive quantum-mechanical (QM) methods. Here, we introduce an equivariant graph neural network (GNN) to address this issue. The proposed model predicts atomic multipoles up to the quadrupole, circumventing the need for expensive QM computations. By using an equivariant architecture, the model enforces the correct symmetry by design without relying on local reference frames. The GNN reproduces the electrostatic potential of various systems with high fidelity. Possible uses for such an approach include the separate treatment of long-range interactions in ML potentials, the analysis of electrostatic potential surfaces, and static multipoles in polarizable force fields.