How Accurate Are Simulations and Experiments for the Lattice Energies of Molecular Crystals?

Della Pia, Flaviano; Zen, Andrea; Alfè, Dario; Michaelides, Angelos

doi:10.1103/PhysRevLett.133.046401

Title: How Accurate Are Simulations and Experiments for the Lattice Energies of Molecular Crystals?

Journal Article · 23 July 2024 · Physical Review Letters

DOI: https://doi.org/10.1103/PhysRevLett.133.046401 · OSTI ID:2406278

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Molecular crystals play a central role in a wide range of scientific fields, including pharmaceuticals and organic semiconductor devices. However, they are challenging systems to model accurately with computational approaches because of a delicate interplay of intermolecular interactions such as hydrogen bonding and Van der Waals dispersion forces. Here, by exploiting recent algorithmic developments, we report the first set of diffusion Monte Carlo lattice energies for all 23 molecular crystals in the popular and widely used X23 dataset. Comparisons with previous state-of-the-art lattice energy predictions (on a subset of the dataset) and a careful analysis of experimental sublimation enthalpies reveals that high-accuracy computational methods are now at least as reliable as (computationally derived) experiments for the lattice energies of molecular crystals. Overall, this work demonstrates the feasibility of high-level explicitly correlated electronic structure methods for broad benchmarking studies in complex condensed phase systems, and signposts a route towards closer agreement between experiment and simulation. Published by the American Physical Society 2024

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Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2406278

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 4 Vol. 133; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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