Two-photon absorption and third-harmonic generation of di-alkyl-amino- nitro-stilbene (DANS): A joint experimental and theoretical study

D. Beljonne*, Jean-Luc Bredas, M. Cha, W. E. Torruellas, G. I. Stegeman, J. W. Hofstraat, W. H.G. Horsthuis, G. R. Möhlmann

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

91 Scopus citations

Abstract

The one- and two-photon optical absorption spectra as well as the frequency dependent third-harmonic generation response of a side-chain polymer containing 4-dialkylamino-4′-nitro-stilbene (DANS) as its side group have been measured over a wide range of frequency. A three-state model, based on an intermediate neglect of differential overlap/multireference double-configuration interaction description of the excited states, provides a coherent picture of the dynamic response of DANS, but fails in reproducing the red shift observed when going from the linear to the nonlinear absorption spectra; including vibronic coupling within the Franck-Condon approximation improves the fit.

Original languageEnglish (US)
Pages (from-to)7834-7843
Number of pages10
JournalThe Journal of Chemical Physics
Volume103
Issue number18
DOIs
StatePublished - Jan 1 1995

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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