Variational determination of ground and excited-state two-electron reduced density matrices in the doubly occupied configuration space: A dispersion operator approach
This work implements a variational determination of the elements of two-electron reduced density matrices corresponding to the ground and excited states of N-electron interacting systems based on the dispersion operator technique. The procedure extends the previously reported proposal [Nakata et al....
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Veröffentlicht in: | The Journal of chemical physics 2021-06, Vol.154 (22), p.224104-224104 |
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Hauptverfasser: | , , , , , , , , |
Format: | Artikel |
Sprache: | eng |
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Online-Zugang: | Volltext |
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Zusammenfassung: | This work implements a variational determination of the elements of two-electron reduced density matrices corresponding to the ground and excited states of N-electron interacting systems based on the dispersion operator technique. The procedure extends the previously reported proposal [Nakata et al., J. Chem. Phys. 125, 244109 (2006)] to two-particle interaction Hamiltonians and N-representability conditions for the two-, three-, and four-particle reduced density matrices in the doubly occupied configuration interaction space. The treatment has been applied to describe electronic spectra using two benchmark exactly solvable pairing models: reduced Bardeen–Cooper–Schrieffer and Richardson–Gaudin–Kitaev Hamiltonians. The dispersion operator combined with N-representability conditions up to the four-particle reduced density matrices provides excellent results. |
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ISSN: | 0021-9606 1089-7690 |
DOI: | 10.1063/5.0051793 |