Issue 37, 2022

Graph-convolutional neural networks for (QM)ML/MM molecular dynamics simulations

Abstract

To accurately study the chemical reactions in the condensed phase or within enzymes, both quantum-mechanical description and sufficient configurational sampling are required to reach converged estimates. Here, quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations play an important role, providing QM accuracy for the region of interest at a decreased computational cost. However, QM/MM simulations are still too expensive to study large systems on longer time scales. Recently, machine learning (ML) models have been proposed to replace the QM description. The main limitation of these models lies in the accurate description of long-range interactions present in condensed-phase systems. To overcome this issue, a recent workflow has been introduced combining a semi-empirical method (i.e. density functional tight binding (DFTB)) and a high-dimensional neural network potential (HDNNP) in a Δ-learning scheme. This approach has been shown to be capable of correctly incorporating long-range interactions within a cutoff of 1.4 nm. One of the promising alternative approaches to efficiently take long-range effects into account is the development of graph-convolutional neural networks (GCNNs) for the prediction of the potential-energy surface. In this work, we investigate the use of GCNN models – with and without a Δ-learning scheme – for (QM)ML/MM MD simulations. We show that the Δ-learning approach using a GCNN and DFTB as a baseline achieves competitive performance on our benchmarking set of solutes and chemical reactions in water. This method is additionally validated by performing prospective (QM)ML/MM MD simulations of retinoic acid in water and S-adenoslymethionine interacting with cytosine in water. The results indicate that the Δ-learning GCNN model is a valuable alternative for the (QM)ML/MM MD simulations of condensed-phase systems.

Graphical abstract: Graph-convolutional neural networks for (QM)ML/MM molecular dynamics simulations

Supplementary files

Article information

Article type
Paper
Submitted
28 Jun 2022
Accepted
30 Aug 2022
First published
15 Sep 2022
This article is Open Access
Creative Commons BY-NC license

Phys. Chem. Chem. Phys., 2022,24, 22497-22512

Graph-convolutional neural networks for (QM)ML/MM molecular dynamics simulations

A. Hofstetter, L. Böselt and S. Riniker, Phys. Chem. Chem. Phys., 2022, 24, 22497 DOI: 10.1039/D2CP02931F

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. You can use material from this article in other publications, without requesting further permission from the RSC, provided that the correct acknowledgement is given and it is not used for commercial purposes.

To request permission to reproduce material from this article in a commercial publication, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party commercial publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements