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  Strictly-correlated-electron approach to excitation energies of dissociating molecules

Cort, L., Nielsen, S. E. B., & van Leeuwen, R. (2019). Strictly-correlated-electron approach to excitation energies of dissociating molecules. Physical Review A, 99(2): 022501. doi:10.1103/PhysRevA.99.022501.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0003-00D1-0 Version Permalink: http://hdl.handle.net/21.11116/0000-0003-00D5-C
Genre: Journal Article

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https://dx.doi.org/10.1103/PhysRevA.99.022501 (Publisher version)
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 Creators:
Cort, L.1, Author
Nielsen, S. E. B.2, 3, Author              
van Leeuwen, R.1, Author
Affiliations:
1Department of Physics, Nanoscience Center P.O. Box 35 FI-40014 University of Jyväskylä, Finland, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science, ou_persistent22              

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 Abstract: In this work we consider a numerically solvable model of a two-electron diatomic molecule to study a recently proposed approximation based on the density functional theory of so-called strictly correlated electrons (SCE). We map out the full two-particle wave function for a wide range of bond distances and interaction strengths and obtain analytic results for the two-particle states and eigenenergies in various limits of strong and weak interactions, and in the limit of large bond distance. We then study the so-called Hartree-exchange-correlation (Hxc) kernel of time-dependent density functional theory which is a key ingredient in calculating excitation energies. We study an approximation based on adiabatic SCE (ASCE) theory which was shown to display a particular feature of the exact Hxc kernel, namely, a spatial divergence as function of the bond distance. This makes the ASCE kernel a candidate for correcting a notorious failure of the commonly used adiabatic local density approximation (ALDA) in the calculation of excitation energies of dissociating molecules. Unlike the ALDA, we obtain nonzero excitation energies from the ASCE kernel in the dissociation regime but they do not correspond to those of the true spectrum unless the interaction strength is taken to be very large such that the SCE theory has the right regime of validity, in which case the excitation energies become exact and represent the so-called zero-point oscillations of the strictly correlated electrons. The commonly studied physical dissociation regime, namely, large molecular separation at intermediate interaction strength, therefore remains a challenge for density functional approximations based on SCE theory.

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Language(s): eng - English
 Dates: 2018-12-142019-02-042019-02-04
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1103/PhysRevA.99.022501
arXiv: 1901.05266
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Title: Physical Review A
  Other : Physical Review A: Atomic, Molecular, and Optical Physics
  Other : Phys. Rev. A
Source Genre: Journal
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Publ. Info: New York, NY : American Physical Society
Pages: - Volume / Issue: 99 (2) Sequence Number: 022501 Start / End Page: - Identifier: ISSN: 1050-2947
CoNE: https://pure.mpg.de/cone/journals/resource/954925225012_2