Issue 32, 2021

A transferable active-learning strategy for reactive molecular force fields


Predictive molecular simulations require fast, accurate and reactive interatomic potentials. Machine learning offers a promising approach to construct such potentials by fitting energies and forces to high-level quantum-mechanical data, but doing so typically requires considerable human intervention and data volume. Here we show that, by leveraging hierarchical and active learning, accurate Gaussian Approximation Potential (GAP) models can be developed for diverse chemical systems in an autonomous manner, requiring only hundreds to a few thousand energy and gradient evaluations on a reference potential-energy surface. The approach uses separate intra- and inter-molecular fits and employs a prospective error metric to assess the accuracy of the potentials. We demonstrate applications to a range of molecular systems with relevance to computational organic chemistry: ranging from bulk solvents, a solvated metal ion and a metallocage onwards to chemical reactivity, including a bifurcating Diels–Alder reaction in the gas phase and non-equilibrium dynamics (a model SN2 reaction) in explicit solvent. The method provides a route to routinely generating machine-learned force fields for reactive molecular systems.

Graphical abstract: A transferable active-learning strategy for reactive molecular force fields

Supplementary files

Article information

Article type
Edge Article
31 Mar 2021
04 Jul 2021
First published
05 Jul 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2021,12, 10944-10955

A transferable active-learning strategy for reactive molecular force fields

T. A. Young, T. Johnston-Wood, V. L. Deringer and F. Duarte, Chem. Sci., 2021, 12, 10944 DOI: 10.1039/D1SC01825F

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