Work

Joint approximate diagonalization approach to quasiparticle self-consistent GW calculations

Year: 2025

Type: article

Abstract: We introduce an alternative route to quasiparticle self-consistent GW calculations (qsGW) on the basis of a joint approximate diagonalization of the one-body GW Green's functions G(εnQP) taken at the input quasiparticle energies. Such an approach allows working with the full dynamical self-energy, without approximating the latter by a symmetrized static form as in the standard qsGW scheme. Calculations on the GW100 molecular test set lead, nevertheless, to a good agreement, at the 60 meV mean-absolute-error accuracy on the ionization potential, with respect to the conventional qsGW approach. We show further that constructing the density matrix from the full Green's function as in the fully self-consistent scGW scheme, and not from the occupied quasiparticle one-body orbitals, allows obtaining a scheme intermediate between the qsGW and scGW approaches, closer to coupled-cluster reference values.

Source: The Journal of Chemical Physics

DOI: 10.1063/5.0250929

Authors: Ivan Duchemin, Xavier Blase

Institutions: Commissariat à l'Énergie Atomique et aux Énergies Alternatives, CEA Grenoble, Institut de Recherche Interdisciplinaire de Grenoble, Centre National de la Recherche Scientifique, Institut Néel

Language: English

Topic: Advanced Chemical Physics Studies

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: green

Funders: Agence Nationale de la Recherche, Grand Équipement National De Calcul Intensif

Awards: G3440483028, Towards Accurate Excited-State Geometries with the Bethe-Salpeter Formalism, G5186824767, G8880582076