Finite lifetime effects on the polarizability within time-dependent density-functional theory

L. Jensen, J. Autschbach, George C Schatz

Research output: Contribution to journalArticle

126 Citations (Scopus)

Abstract

We present an implementation for considering finite lifetime of the electronic excited states into linear-response theory within time-dependent density-functional theory. The lifetime of the excited states is introduced by a common phenomenological damping factor. The real and imaginary frequency-dependent polarizabilities can thus be calculated over a broad range of frequencies. This allows for the study of linear-response properties both in the resonance and nonresonance cases. The method is complementary to the standard approach of calculating the excitation energies from the poles of the polarizability. The real and imaginary polarizabilities can then be calculated in any specific energy range of interest, in contrast to the excitation energies which are usually solved only for the lowest electronic states. We have verified the method by investigating the photoabsorption properties of small alkali clusters. For these systems, we have calculated the real and imaginary polarizabilities in the energy range of 1-4 eV and compared these with excitation energy calculations. The results showed good agreement with both previous theoretical and experimental results.

Original languageEnglish
Article number224115
JournalJournal of Chemical Physics
Volume122
Issue number22
DOIs
Publication statusPublished - Jun 8 2005

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Excitation energy
Density functional theory
density functional theory
Excited states
life (durability)
excitation
Alkalies
Electronic states
energy
Poles
nonresonance
Damping
photoabsorption
electronics
alkalies
poles
damping

ASJC Scopus subject areas

  • Atomic and Molecular Physics, and Optics

Cite this

Finite lifetime effects on the polarizability within time-dependent density-functional theory. / Jensen, L.; Autschbach, J.; Schatz, George C.

In: Journal of Chemical Physics, Vol. 122, No. 22, 224115, 08.06.2005.

Research output: Contribution to journalArticle

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