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Title: Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices

Abstract

Recently, it was shown that the calculation of quasiparticle energies using the G0W0 approximation can be performed without computing explicitly any virtual electronic states, by expanding the Green function and screened Coulomb interaction in terms of the eigenstates of the static dielectric matrix. Avoiding the evaluation of virtual electronic states leads to improved efficiency and ease of convergence of G0W0 calculations. Here, we propose a further improvement of the efficiency of these calculations, based on an approximation of density-density response functions of molecules and solids. The approximation relies on the calculation of a subset of eigenvectors of the dielectric matrix using the kinetic operator instead of the full Hamiltonian, and it does not lead to any substantial loss of accuracy for the quasiparticle energies. The computational savings introduced by this approximation depend on the system, and they become more substantial as the number of electrons increases.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering
  2. Univ. of Chicago, IL (United States). Pritzker School of Molecular Engineering; Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1595951
Alternate Identifier(s):
OSTI ID: 1577886
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 22; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yang, Han, Govoni, Marco, and Galli, Giulia. Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices. United States: N. p., 2019. Web. doi:10.1063/1.5126214.
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Yang, Han, Govoni, Marco, & Galli, Giulia. Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices. United States. https://doi.org/10.1063/1.5126214
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Yang, Han, Govoni, Marco, and Galli, Giulia. Sat . "Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices". United States. https://doi.org/10.1063/1.5126214. https://www.osti.gov/servlets/purl/1595951.
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@article{osti_1595951,
title = {Improving the efficiency of G0W0 calculations with approximate spectral decompositions of dielectric matrices},
author = {Yang, Han and Govoni, Marco and Galli, Giulia},
abstractNote = {Recently, it was shown that the calculation of quasiparticle energies using the G0W0 approximation can be performed without computing explicitly any virtual electronic states, by expanding the Green function and screened Coulomb interaction in terms of the eigenstates of the static dielectric matrix. Avoiding the evaluation of virtual electronic states leads to improved efficiency and ease of convergence of G0W0 calculations. Here, we propose a further improvement of the efficiency of these calculations, based on an approximation of density-density response functions of molecules and solids. The approximation relies on the calculation of a subset of eigenvectors of the dielectric matrix using the kinetic operator instead of the full Hamiltonian, and it does not lead to any substantial loss of accuracy for the quasiparticle energies. The computational savings introduced by this approximation depend on the system, and they become more substantial as the number of electrons increases.},
doi = {10.1063/1.5126214},
journal = {Journal of Chemical Physics},
number = 22,
volume = 151,
place = {United States},
year = {2019},
month = {12}
}
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