Fourier analysis of the femtosecond hyper-Rayleigh scattering signal from ionic fluorescent hemicyanine dyes

Koen Clays*, Kurt Wostyn, Geert Olbrechts, André Persoons, Akira Watanabe, Kyoko Nogi, Xuan Ming Duan, Shuji Okada, Hidetosbi Oikawa, Hachiro Nakanishi, Henryk Vogel, David Beljonne, Jean Luc Brédas

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

76 Scopus citations


A series of five fluorescent and ionic dimethylamino stilbazolium homologues with increasing conjugation length (from ethenyl to decapentaenyl) is investigated by high-frequency, amplitude-modulated femtosecond hyper-Rayleigh scattering at 1300 nm. A hyperpolarizability value that is not overestimated by the presence of a multiphoton fluorescence contribution is obtained from the Fourier analysis of the hyper-Rayleigh scattering signal. The demodulation curve (decrease of Fourier amplitude versus modulation frequency) is characterized by both the hyperpolarizability value and the fluorescence decay parameters. The fluorescence decay parameters are accurately determined independently by single-photon counting. A detailed analysis of the fluorescence decay parameters from the hyper-Rayleigh scattering demodulation curve and of their relation to the fluorescence decay parameters obtained from single-photon counting experiments is presented. The inherent hyperpolarizability value for these chromophores shows a maximum of (2045 ± 35) × 10-30 esu or (760 ± 13) × 10-50 C3 m3 J-2 for the hexatrienyl conjugation length. A comparison with theoretical calculations suggests the importance of trans-cis isomerization in the excited state.

Original languageEnglish (US)
Pages (from-to)256-265
Number of pages10
JournalJournal of the Optical Society of America B: Optical Physics
Issue number2
StatePublished - Feb 2000
Externally publishedYes

ASJC Scopus subject areas

  • Statistical and Nonlinear Physics
  • Atomic and Molecular Physics, and Optics


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