Regularized by Physics: Graph Neural Network Parametrized Potentials for the Description of Intermolecular Interactions
Open access
Date
2023-01-24Type
- Journal Article
Abstract
Simulations of molecular systems using electronic structure methods are still not feasible for many systems of biological importance. As a result, empirical methods such as force fields (FF) have become an established tool for the simulation of large and complex molecular systems. The parametrization of FF is, however, time-consuming and has traditionally been based on experimental data. Recent years have therefore seen increasing efforts to automatize FF parametrization or to replace FF with machine-learning (ML) based potentials. Here, we propose an alternative strategy to parametrize FF, which makes use of ML and gradient-descent based optimization while retaining a functional form founded in physics. Using a predefined functional form is shown to enable interpretability, robustness, and efficient simulations of large systems over long time scales. To demonstrate the strength of the proposed method, a fixed-charge and a polarizable model are trained on ab initio potential-energy surfaces. Given only information about the constituting elements, the molecular topology, and reference potential energies, the models successfully learn to assign atom types and corresponding FF parameters from scratch. The resulting models and parameters are validated on a wide range of experimentally and computationally derived properties of systems including dimers, pure liquids, and molecular crystals. Show more
Permanent link
https://doi.org/10.3929/ethz-b-000600524Publication status
publishedExternal links
Journal / series
Journal of Chemical Theory and ComputationVolume
Pages / Article No.
Publisher
American Chemical SocietyRelated publications and datasets
Is new version of: https://doi.org/10.3929/ethz-b-000550373
More
Show all metadata