Dispersion XDM with Hybrid Functionals: Delocalization Error and Halogen Bonding in Molecular Crystals

Journal of Chemical Theory and Computation
Alberto Otero-de-la-RozaErin R Johnson

Abstract

The accurate calculation of relative lattice energies of molecular crystals is important in polymorph ranking and crystal structure prediction. Delocalization error has been shown to affect calculated intermolecular binding energies in DFT and is similarly expected to affect the lattice energies of some classes of molecular crystals. In this work, we explore the use of dispersion-corrected hybrid functionals in the planewave-pseudopotentials approach to reduce delocalization error. We combine several hybrid functionals with the exchange-hole dipole moment (XDM) model for dispersion and show that they generally outperform GGA functionals in the calculation of both gas-phase binding energies and molecular crystal lattice energies. We apply the resulting XDM-corrected functionals to four halogen-bonded crystals: Cl2, Br2, I2, and ICl. GGA functionals severely overestimate their lattice energies, while hybrid functionals give accurate values. The preference of GGA functionals for monatomic structures in the Br2 and Cl2 crystals is also explained. Finally, we apply a recently developed method to calculate Bader's delocalization indices to examine the extent of intermolecular delocalization in the halogen molecular crystals. It is sh...Continue Reading

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Citations

Apr 15, 2020·Physical Chemistry Chemical Physics : PCCP·A Otero-de-la-RozaErin R Johnson
Aug 11, 2020·The Journal of Chemical Physics·A Otero-de-la-Roza, Erin R Johnson
Sep 12, 2020·International Journal of Molecular Sciences·Nicholas J Thornton, Tanja van Mourik
Dec 16, 2020·The Journal of Chemical Physics·Cameron Cook, Gregory J O Beran
Apr 22, 2021·Journal of Chemical Theory and Computation·Nisha MehtaLars Goerigk
Jul 10, 2021·The Journal of Chemical Physics·Alastair J A PriceErin R Johnson
Aug 14, 2020·Journal of Chemical Theory and Computation·D ChakrabortyT Thonhauser

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