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Pré-Publication, Document De Travail Année : 2015

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 Be atom and four small molecules (N$_2$, CO$_2$, H$_2$CO, and C$_2$H$_4$). The results suggest that the addition of the long-range second-order Bethe-Salpeter correlation kernel overall slightly improves the excitation energies.
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Dates et versions

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

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Citer

Elisa Rebolini, Julien Toulouse. Range-separated time-dependent density-functional theory with a frequency-dependent second-order Bethe-Salpeter correlation kernel. 2015. ⟨hal-01184145v2⟩
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