English

Benchmarking GW against exact diagonalization for semi-empirical models

Mesoscale and Nanoscale Physics 2013-11-22 v1

Abstract

We calculate groundstate total energies and single-particle excitation energies of seven pi conjugated molecules described with the semi-empirical Pariser-Parr-Pople (PPP) model using self-consistent many-body perturbation theory at the GW level and exact diagonalization. For the total energies GW captures around 65% of the groundstate correlation energy. The lowest lying excitations are overscreened by GW leading to an underestimation of electron affinities and ionization potentials by approximately 0.15 eV corresponding to 2.5%. One-shot G_0W_0 calculations starting from Hartree-Fock reduce the screening and improve the low-lying excitation energies. The effect of the GW self-energy on the molecular excitation energies is shown to be similar to the inclusion of final state relaxations in Hartree-Fock theory. We discuss the break down of the GW approximation in systems with short range interactions (Hubbard models) where correlation effects dominate over screening/relaxation effects. Finally we illustrate the important role of the derivative discontinuity of the true exchange-correlation functional by computing the exact Kohn-Sham levels of benzene.

Keywords

Cite

@article{arxiv.0912.0801,
  title  = {Benchmarking GW against exact diagonalization for semi-empirical models},
  author = {K. Kaasbjerg and K. S. Thygesen},
  journal= {arXiv preprint arXiv:0912.0801},
  year   = {2013}
}

Comments

9 pages, 5 figures, accepted for publication in Phys. Rev. B

R2 v1 2026-06-21T14:19:32.712Z