Excited states from range-separated density-functional perturbation theory
We explore the possibility of calculating electronic excited states by using perturbation theory along a range-separated adiabatic connection. Starting from the energies of a partially interacting Hamiltonian, a first-order correction is defined with two variants of perturbation theory: a straightfo...
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| Format: | Article |
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Taylor and Francis
2015
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| Online Access: | https://eprints.nottingham.ac.uk/31094/ |
| _version_ | 1848794126707851264 |
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| author | Rebolini, Elisa Toulouse, Julien Teale, Andrew M. Helgaker, Trygve Savin, Andreas |
| author_facet | Rebolini, Elisa Toulouse, Julien Teale, Andrew M. Helgaker, Trygve Savin, Andreas |
| author_sort | Rebolini, Elisa |
| building | Nottingham Research Data Repository |
| collection | Online Access |
| description | We explore the possibility of calculating electronic excited states by using perturbation theory along a range-separated adiabatic connection. Starting from the energies of a partially interacting Hamiltonian, a first-order correction is defined with two variants of perturbation theory: a straightforward perturbation theory, and an extension of the Görling-Levy one that has the advantage of keeping the ground-state density constant at each order in the perturbation. Only the first, simpler, variant is tested here on the helium and beryllium atoms and on the hydrogen molecule. The first-order correction within this perturbation theory improves significantly the total ground- and excited-state energies of the different systems. However, the excitation energies mostly deteriorate with respect to the zeroth-order ones, which may be explained by the fact that the ionization energy is no longer correct for all interaction strengths. The second (Görling-Levy) variant of the perturbation theory should improve these results but has not been tested yet along the range-separated adiabatic connection. |
| first_indexed | 2025-11-14T19:11:14Z |
| format | Article |
| id | nottingham-31094 |
| institution | University of Nottingham Malaysia Campus |
| institution_category | Local University |
| last_indexed | 2025-11-14T19:11:14Z |
| publishDate | 2015 |
| publisher | Taylor and Francis |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | nottingham-310942020-05-04T17:02:34Z https://eprints.nottingham.ac.uk/31094/ Excited states from range-separated density-functional perturbation theory Rebolini, Elisa Toulouse, Julien Teale, Andrew M. Helgaker, Trygve Savin, Andreas We explore the possibility of calculating electronic excited states by using perturbation theory along a range-separated adiabatic connection. Starting from the energies of a partially interacting Hamiltonian, a first-order correction is defined with two variants of perturbation theory: a straightforward perturbation theory, and an extension of the Görling-Levy one that has the advantage of keeping the ground-state density constant at each order in the perturbation. Only the first, simpler, variant is tested here on the helium and beryllium atoms and on the hydrogen molecule. The first-order correction within this perturbation theory improves significantly the total ground- and excited-state energies of the different systems. However, the excitation energies mostly deteriorate with respect to the zeroth-order ones, which may be explained by the fact that the ionization energy is no longer correct for all interaction strengths. The second (Görling-Levy) variant of the perturbation theory should improve these results but has not been tested yet along the range-separated adiabatic connection. Taylor and Francis 2015-02-18 Article PeerReviewed Rebolini, Elisa, Toulouse, Julien, Teale, Andrew M., Helgaker, Trygve and Savin, Andreas (2015) Excited states from range-separated density-functional perturbation theory. Molecular Physics, 113 (13-14). pp. 1740-1749. ISSN 0026-8976 http://www.tandfonline.com/doi/full/10.1080/00268976.2015.1011248 doi:10.1080/00268976.2015.1011248 doi:10.1080/00268976.2015.1011248 |
| spellingShingle | Rebolini, Elisa Toulouse, Julien Teale, Andrew M. Helgaker, Trygve Savin, Andreas Excited states from range-separated density-functional perturbation theory |
| title | Excited states from range-separated density-functional perturbation theory |
| title_full | Excited states from range-separated density-functional perturbation theory |
| title_fullStr | Excited states from range-separated density-functional perturbation theory |
| title_full_unstemmed | Excited states from range-separated density-functional perturbation theory |
| title_short | Excited states from range-separated density-functional perturbation theory |
| title_sort | excited states from range-separated density-functional perturbation theory |
| url | https://eprints.nottingham.ac.uk/31094/ https://eprints.nottingham.ac.uk/31094/ https://eprints.nottingham.ac.uk/31094/ |