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  5. Combining the Δ-self-consistent-field and GW methods for predicting core electron binding energies in periodic solids
 
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Combining the Δ-self-consistent-field and GW methods for predicting core electron binding energies in periodic solids
File(s)
acs.jctc.3c00121.pdf (1.89 MB)
Published version
Author(s)
Kahk, J Matthias
Lischner, Johannes
Type
Journal Article
Abstract
For the computational prediction of core electron binding energies in solids, two distinct kinds of modeling strategies have been pursued: the Δ-Self-Consistent-Field method based on density functional theory (DFT), and the GW method. In this study, we examine the formal relationship between these two approaches and establish a link between them. The link arises from the equivalence, in DFT, between the total energy difference result for the first ionization energy, and the eigenvalue of the highest occupied state, in the limit of infinite supercell size. This link allows us to introduce a new formalism, which highlights how in DFT─even if the total energy difference method is used to calculate core electron binding energies─the accuracy of the results still implicitly depends on the accuracy of the eigenvalue at the valence band maximum in insulators, or at the Fermi level in metals. We examine whether incorporating a quasiparticle correction for this eigenvalue from GW theory improves the accuracy of the calculated core electron binding energies, and find that the inclusion of vertex corrections is required for achieving quantitative agreement with experiment.
Date Issued
2023-06-13
Date Acceptance
2023-05-01
Citation
Journal of Chemical Theory and Computation, 2023, 19 (11), pp.3276-3283
URI
http://hdl.handle.net/10044/1/104740
URL
https://pubs.acs.org/doi/10.1021/acs.jctc.3c00121
DOI
https://www.dx.doi.org/10.1021/acs.jctc.3c00121
ISSN
1549-9618
Publisher
American Chemical Society
Start Page
3276
End Page
3283
Journal / Book Title
Journal of Chemical Theory and Computation
Volume
19
Issue
11
Copyright Statement
© 2023 The Authors. Published by American Chemical Society. This work is published under a CC BY licence.
License URL
http://creativecommons.org/licenses/by/4.0/
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/37163299
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2023-05-10
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