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Hierarchical machine learning of potential energy surfaces.

Published version
Peer-reviewed

Type

Article

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Authors

Abstract

We present hierarchical machine learning (hML) of highly accurate potential energy surfaces (PESs). Our scheme is based on adding predictions of multiple Δ-machine learning models trained on energies and energy corrections calculated with a hierarchy of quantum chemical methods. Our (semi-)automatic procedure determines the optimal training set size and composition of each constituent machine learning model, simultaneously minimizing the computational effort necessary to achieve the required accuracy of the hML PES. Machine learning models are built using kernel ridge regression, and training points are selected with structure-based sampling. As an illustrative example, hML is applied to a high-level ab initio CH3Cl PES and is shown to significantly reduce the computational cost of generating the PES by a factor of 100 while retaining similar levels of accuracy (errors of ∼1 cm-1).

Description

Keywords

51 Physical Sciences, 34 Chemical Sciences, 3406 Physical Chemistry, Networking and Information Technology R&D (NITRD), Machine Learning and Artificial Intelligence

Journal Title

J Chem Phys

Conference Name

Journal ISSN

0021-9606
1089-7690

Volume Title

152

Publisher

AIP Publishing

Rights

All rights reserved