Regularized and Opposite Spin-Scaled Functionals from Møller–Plesset Adiabatic Connection─Higher Accuracy at Lower Cost
Kimberly J. Daas, Derk P. Kooi, Nina C. Peters, Eduardo Fabiano, Fabio Della Sala, Paola Gori‐Giorgi, Stefan Vuckovic
Abstract
Noncovalent interactions (NCIs) play a crucial role in biology, chemistry, material science, and everything in between. To improve pure quantum-chemical simulations of NCIs, we propose a methodology for constructing approximate correlation energies by combining an interpolation along the Møller–Plesset adiabatic connection (MP AC) with a regularization and spin-scaling strategy applied to MP2 correlation energies. This combination yields c os κ os -SPL2, which exhibits superior accuracy for NCIs compared to any of the individual strategies. With the N 4 formal scaling, c os κ os -SPL2 is competitive or often outperforms more expensive dispersion-corrected double hybrids for NCIs. The accuracy of c os κ os -SPL2 particularly shines for anionic halogen bonded complexes, where it surpasses standard dispersion-corrected DFT by a factor of 3 to 5.