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Accurate intermolecular interactions at dramatically reduced cost: XPol+SAPT with empirical dispersion

K. U. Lao and J. M. Herbert
J. Phys. Chem. Lett. 3, 3241–3248

Abstract

An efficient, monomer-based electronic structure method is introduced for computing noncovalent interactions in molecular and ionic clusters. It builds upon our explicit polarization plus symmetry-adapted perturbation theory approach, XPol+SAPT (XPS), but replaces the problematic and expensive sum-over-states dispersion terms with empirical potentials. This modification reduces the scaling from O(N5) to O(N3) with respect to monomer size, and also facilitates the use of Kohn-Sham density functional theory (KS-DFT) as a low-cost means to capture intramolecular electron correlation. The accuracy of the resulting method [XPS(KS)+D], in conjunction with a double-ζ basis set, is superior to MP2-type methods extrapolated to the basis-set limit, with a mean unsigned error of 0.27 kcal/mol for the S66 data set. XPS(KS)+D yields accurate potential energy curves for a variety of challenging systems. As compared to traditional DFT-SAPT methods, it removes the limitation to dimers and extends SAPT-based methodology to many-body systems.

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