Range-separated time-dependent density-functional theory with a frequency-dependent second-order Bethe-Salpeter correlation kernel - Sorbonne Université Accéder directement au contenu
Article Dans Une Revue Journal of Chemical Physics Année : 2016

Range-separated time-dependent density-functional theory with a frequency-dependent second-order Bethe-Salpeter correlation kernel

Résumé

We present a range-separated linear-response time-dependent density-functional theory (TDDFT) which combines a density-functional approximation for the short-range response kernel and a frequency-dependent second-order Bethe-Salpeter approximation for the long-range response kernel. This approach goes beyond the adiabatic approximation usually used in linear-response TDDFT and aims at improving the accuracy of calculations of electronic excitation energies of molecular systems. A detailed derivation of the frequency-dependent second-order Bethe-Salpeter correlation kernel is given using many-body Green-function theory. Preliminary tests of this range-separated TDDFT method are presented for the calculation of excitation energies of the He and Be atoms and small molecules (H2, N2, CO2, H2CO, and C2H4). The results suggest that the addition of the long-range second-order Bethe-Salpeter correlation kernel overall slightly improves the excitation energies.
Fichier principal
Vignette du fichier
main.pdf (255.86 Ko) Télécharger le fichier
Origine : Fichiers produits par l'(les) auteur(s)
Loading...

Dates et versions

hal-01184145 , version 1 (12-08-2015)
hal-01184145 , version 2 (13-10-2015)
hal-01184145 , version 3 (15-02-2016)

Identifiants

Citer

Elisa Rebolini, Julien Toulouse. Range-separated time-dependent density-functional theory with a frequency-dependent second-order Bethe-Salpeter correlation kernel. Journal of Chemical Physics, 2016, 144, pp.094107. ⟨10.1063/1.4943003⟩. ⟨hal-01184145v3⟩
165 Consultations
235 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More