English

Regularized and Opposite spin-scaled functionals from M{\o}ller-Plesset adiabatic connection -- higher accuracy at lower cost

Chemical Physics 2023-07-11 v2

Abstract

Non-covalent 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 M{\o}ller adiabatic connection (MP AC) with a regularization and spin-scaling strategy applied to MP2 correlation energies. This combination yields cosκosc_{\rm os}\kappa_{\rm os}-SPL2, which exhibits superior accuracy for NCIs compared to any of the individual strategies. With the N4N^4 formal scaling, cosκosc_{\rm os}\kappa_{\rm os}-SPL2, is competitive or often outperforms more expensive dispersion-corrected double hybrids for NCIs.The accuracy of cosκosc_{\rm os}\kappa_{\rm os}-SPL2 particularly shines for anionic halogen bonded complexes, where it surpasses standard dispersion-corrected DFT by a factor of 3 to 5.

Keywords

Cite

@article{arxiv.2307.02715,
  title  = {Regularized and Opposite spin-scaled functionals from M{\o}ller-Plesset adiabatic connection -- higher accuracy at lower cost},
  author = {Kimberly J. Daas and Derk P. Kooi and Nina C. Peters and Eduardo Fabiano and Fabio Della Sala and Paola Gori-Giorgi and Stefan Vuckovic},
  journal= {arXiv preprint arXiv:2307.02715},
  year   = {2023}
}

Comments

12 pages + 5 SI, 8 figures + 6 SI

R2 v1 2026-06-28T11:23:17.773Z