Excited-State-Specific Kohn-Sham Formalism for the Asymmetric Hubbard Dimer - Fédération de recherche « Matière et interactions »
Pré-Publication, Document De Travail Année : 2024

Excited-State-Specific Kohn-Sham Formalism for the Asymmetric Hubbard Dimer

Résumé

Building on our recent study [https://doi.org/10.1021/acs.jpclett.3c02052, J. Phys. Chem. Lett. 14, 8780 (2023)], we explore the generalization of the ground-state Kohn-Sham (KS) formalism of density-functional theory (DFT) to the (singlet) excited states of the asymmetric Hubbard dimer at half-filling. While we found that the KS-DFT framework can be straightforwardly generalized to the highest-lying doubly-excited state, the treatment of the first excited state presents significant challenges. Specifically, using a density-fixed adiabatic connection, we show that the density of the first excited state lacks non-interacting $v$-representability. However, by employing an analytic continuation of the adiabatic path, we demonstrate that the density of the first excited state can be generated by a complex-valued external potential in the non-interacting case. More practically, by performing state-specific KS calculations with exact and approximate correlation functionals -- each state possessing a distinct correlation functional -- we observe that spurious stationary solutions of the KS equations may arise due to the approximate nature of the functional.
Fichier principal
Vignette du fichier
2412.14945v1.pdf (1.18 Mo) Télécharger le fichier
Origine Fichiers produits par l'(les) auteur(s)

Dates et versions

hal-04850869 , version 1 (20-12-2024)

Identifiants

Citer

Pierre-François Loos, Sara Giarrusso. Excited-State-Specific Kohn-Sham Formalism for the Asymmetric Hubbard Dimer. 2024. ⟨hal-04850869⟩
0 Consultations
0 Téléchargements

Altmetric

Partager

More