Woods, N. D., Entwistle, M. T. and Godby, R. W. orcid.org/0000-0002-1012-4176 (2021) Accurate total energies from the adiabatic-connection fluctuation-dissipation theorem. Physical Review B. 125126. ISSN 2469-9969
Abstract
In the context of inhomogeneous one-dimensional finite systems, recent numerical advances [Phys. Rev. B 103, 125155 (2021)2469-995010.1103/PhysRevB.103.125155] allow us to compute the exact coupling-constant dependent exchange-correlation kernel fxcλ(x,x′,ω) within linear response time-dependent density-functional theory. This permits an improved understanding of ground-state total energies derived from the adiabatic-connection fluctuation-dissipation theorem (ACFDT). We consider both one-shot and self-consistent ACFDT calculations, and demonstrate that chemical accuracy is reliably preserved when the frequency dependence in the exact functional fxc[n](ω=0) is neglected. This performance is understood on the grounds that the exact fxc[n] varies slowly over the most relevant ω range (but not in general), and hence the spatial structure in fxc[n](ω=0) is able to largely remedy the principal issue in the present context: self-interaction (examined from the perspective of the exchange-correlation hole). Moreover, we find that the implicit orbitals contained within a self-consistent ACFDT calculation utilizing the adiabatic exact kernel fxc[n](ω=0) are remarkably similar to the exact Kohn-Sham orbitals, thus further establishing that the majority of the physics required to capture the ground-state total energy resides in the spatial dependence of fxc[n] at ω=0.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | Funding Information: The authors thank Micheal Hutcheon for helpful discussions. N.D.W. is supported by the EPSRC Centre for Doctoral Training in Computational Methods for Materials Science for funding under Grant No. EP/L015552/1. We are grateful for computational support from the UK national high performance computing service, ARCHER, through the UKCP consortium under EPSRC Grant No. EP/P022596/1. © 2021 American Physical Society. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details |
Dates: |
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Institution: | The University of York |
Academic Units: | The University of York > Faculty of Sciences (York) > Physics (York) |
Depositing User: | Pure (York) |
Date Deposited: | 08 Oct 2021 08:30 |
Last Modified: | 24 Oct 2024 00:13 |
Published Version: | https://doi.org/10.1103/PhysRevB.104.125126 |
Status: | Published |
Refereed: | Yes |
Identification Number: | 10.1103/PhysRevB.104.125126 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:179016 |
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Description: Accurate total energies from the adiabatic-connection fluctuation-dissipation theorem