Combining localized orbital scaling correction and Bethe-Salpeter equation for accurate excitation energies.

Journal Article (Journal Article)

We applied localized orbital scaling correction (LOSC) in Bethe-Salpeter equation (BSE) to predict accurate excitation energies for molecules. LOSC systematically eliminates the delocalization error in the density functional approximation and is capable of approximating quasiparticle (QP) energies with accuracy similar to or better than GW Green's function approach and with much less computational cost. The QP energies from LOSC, instead of commonly used G0 W0 and evGW, are directly used in BSE. We show that the BSE/LOSC approach greatly outperforms the commonly used BSE/G0 W0 approach for predicting excitations with different characters. For the calculations of Truhlar-Gagliardi test set containing valence, charge transfer, and Rydberg excitations, BSE/LOSC with the Tamm-Dancoff approximation provides a comparable accuracy to time-dependent density functional theory (TDDFT) and BSE/evGW. For the calculations of Stein CT test set and Rydberg excitations of atoms, BSE/LOSC considerably outperforms both BSE/G0 W0 and TDDFT approaches with a reduced starting point dependence. BSE/LOSC is, thus, a promising and efficient approach to calculate excitation energies for molecular systems.

Full Text

Duke Authors

Cited Authors

  • Li, J; Jin, Y; Su, NQ; Yang, W

Published Date

  • April 2022

Published In

Volume / Issue

  • 156 / 15

Start / End Page

  • 154101 -

PubMed ID

  • 35459294

Pubmed Central ID

  • PMC9033305

Electronic International Standard Serial Number (EISSN)

  • 1089-7690

International Standard Serial Number (ISSN)

  • 0021-9606

Digital Object Identifier (DOI)

  • 10.1063/5.0087498

Language

  • eng