Machine-learnt fragment-based energies for crystal structure prediction

Abstract

Crystal structure prediction involves a search of a complex configurational space for local minima corresponding to stable crystal structures, which can be performed efficiently using atom-atom force fields for the assessment of intermolecular interactions. However, for challenging systems, the limitations in the accuracy of force fields prevents a reliable assessment of the relative thermodynamic stability of potential structures, while the cost of fully quantum mechanical approaches can limit applications of the methods. We present a method to rapidly improve force field lattice energies by correcting two-body interactions with a higher level of theory in a fragment-based approach, and predicting these corrections with machine learning. Corrected lattice energies with commonly used density functionals and second order perturbation theory (MP2) all significantly improve the ranking of experimentally known polymorphs where the rigid molecule model is applicable. The relative lattice energies of known polymorphs are also found to systematically improve with the fragment corrections. Predicting two-body interactions with atom-centered symmetry functions in a Gaussian process is found to give highly accurate results using as little as 10-20% of the data for training, reducing the cost of the energy correction by up to an order of magnitude. The machine learning approach opens up the possibility of more widespread use of fragment-based methods in crystal structure prediction, whose increased accuracy at a low computational cost will benefit applications in areas such as polymorph screening and computer-guided materials discovery.

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Identifiers

ORCID for Chris-Kriton Skylaris: orcid.org/0000-0003-0258-3433

ORCID for Graeme M. Day: orcid.org/0000-0001-8396-2771

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