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  Towards Density Functional Approximations from Coupled Cluster Correlation Energy Densities

Margraf, J. T., Kunkel, C., & Reuter, K. (2019). Towards Density Functional Approximations from Coupled Cluster Correlation Energy Densities. The Journal of Chemical Physics, 150(24): 244116. doi:/10.1063/1.5094788.

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 Creators:
Margraf, Johannes T.1, Author
Kunkel, Christian1, Author
Reuter, Karsten1, Author           
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1Chair for Theoretical Chemistry, Catalysis Research Center, Technische Universität München, ou_persistent22              

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 Abstract: (Semi)local density functional approximations (DFAs) are the workhorse electronic structure methods in condensed matter theory and surface science. The correlation energy density ϵc(r) (a spatial function that yields the correlation energy Ec upon integration) is central to defining such DFAs. Unlike Ec, ϵc(r) is not uniquely defined, however. Indeed, there are infinitely many functions that integrate to the correct Ec for a given electron density ρ. The challenge for constructing useful DFAs is thus to find a suitable connection between ϵc(r) and ρ. Herein, we present a new such approach by deriving ϵc(r) directly from the coupled-cluster (CC) energy expression. The corresponding energy densities are analyzed for prototypical two-electron systems. As a proof-of-principle, we construct a semilocal functional to approximate the numerical CC correlation energy densities. Importantly, the energy densities are not simply used as reference data but guide the choice of the functional form, leading to a remarkably simple and accurate correlation functional for the helium isoelectronic series. While the resulting functional is not transferable to many-electron systems (due to a lack of same-spin correlation), these results underscore the potential of the presented approach.

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Language(s): eng - English
 Dates: 2019-03-052019-06-062019-06-282019-06-28
 Publication Status: Issued
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: /10.1063/1.5094788
 Degree: -

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Title: The Journal of Chemical Physics
  Abbreviation : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: 9 Volume / Issue: 150 (24) Sequence Number: 244116 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226