Predictive crystallography at scale: mapping, validating, and learning from 1,000 crystal energy landscapes

Abstract

Computational crystal structure prediction (CSP) is an increasingly powerful technique in materials discovery, due to its ability to reveal trends and permit insight across the possibility space of crystal structures of a candidate molecule, beyond simply the observed structure(s). In this work, we demonstrate the reliability and scalability of CSP methods for small, rigid organic molecules by performing in-depth CSP investigations for over 1000 such compounds, the largest survey of its kind to-date. We show that this highly-efficient force-field-based CSP approach is superbly predictive, locating 99.4\% of observed experimental structures, and ranking a large majority of these (74\%) as among the most stable possible structures (to within uncertainty due to thermal effects). We present two examples of insights such large predicted datasets can permit, examining the space group preferences of organic molecular crystals and rationalising empirical rules concerning the spontaneous resolution of chiral molecules. Finally, we exploit this large and diverse dataset for developing transferable machine-learned energy potentials for the organic solid state, training a neural network lattice energy correction to force field energies that offers substantial improvements to the already impressive energy rankings, and a MACE equivariant message-passing neural network for crystal structure reoptimisation. We conclude that the excellent performance and reliability of the CSP workflow enables the creation of very large datasets of broad utility and explanatory power in materials design.

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Identifiers

ORCID for Christopher R. Taylor: orcid.org/0000-0001-9465-5742

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

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