DFT Accuracy on Crystal Structure Prediction with Machine Learning Interatomic Potentials

Abstract

We present an evaluation of CSP-MACE-{\AA}, a machine learning interatomic potential intended to replace DFT in crystal structure prediction (CSP). We decompose the total energy into separate intramolecular and intermolecular components. For the intramolecular component, we adopt the MACE-POLAR architecture and train it on the OMol25 dataset. The intermolecular component combines three terms: an intermolecular contribution from the MACE-POLAR model, a long-range dispersion term with the functional form of the XDM correction, and a learned delta model trained to reproduce B86bPBE-XDM intermolecular energies. The learned delta model is trained on residual intermolecular targets derived from 50,000 B86bPBE-XDM calculations on molecular crystal structures. On an evaluation set composed of 19 compounds, including a salt, selected from AstraZeneca's previous CSP publications, CSP-MACE-{\AA} achieves performance comparable to PBE DFT with the Neumann-Perrin dispersion correction. On a second evaluation set composed of 28 compounds, including cocrystals and salts, collated from the seven CSP blind tests, CSP-MACE-{\AA} achieves performance close to B86bPBE-XDM DFT. In both evaluation sets, reranking with harmonic free energies substantially improves performance relative to ranking by energy alone. Across our evaluation suite, CSP-MACE-{\AA} is shown to outperform the MACE-POLAR-1 and UMA-OMC foundation models. Lastly, on a set of five compounds, CSP-MACE-{\AA} is shown to capture temperature-dependent trends in the relative stability of polymorphs through estimation of the free energy under the harmonic approximation. By running multiple orders of magnitude faster than DFT, CSP-MACE-{\AA} enables energy and free energy evaluation of far more candidate structures, providing greater confidence when derisking solid forms.