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

doi:10.1364/JOSAB.17.000256

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 journal › Article › peer-review

76 Scopus citations

Abstract

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 language	English (US)
Pages (from-to)	256-265
Number of pages	10
Journal	Journal of the Optical Society of America B: Optical Physics
Volume	17
Issue number	2
DOIs	https://doi.org/10.1364/JOSAB.17.000256
State	Published - Feb 2000
Externally published	Yes

ASJC Scopus subject areas

Statistical and Nonlinear Physics
Atomic and Molecular Physics, and Optics

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Clays, K., Wostyn, K., Olbrechts, G., Persoons, A., Watanabe, A., Nogi, K., Duan, X. M., Okada, S., Oikawa, H., Nakanishi, H., Vogel, H., Beljonne, D., & Brédas, J. L. (2000). Fourier analysis of the femtosecond hyper-Rayleigh scattering signal from ionic fluorescent hemicyanine dyes. Journal of the Optical Society of America B: Optical Physics, 17(2), 256-265. https://doi.org/10.1364/JOSAB.17.000256

@article{355007881cf3464aad0f403fb21b0ee4,

title = "Fourier analysis of the femtosecond hyper-Rayleigh scattering signal from ionic fluorescent hemicyanine dyes",

abstract = "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.",

author = "Koen Clays and Kurt Wostyn and Geert Olbrechts and Andr{\'e} Persoons and Akira Watanabe and Kyoko Nogi and Duan, {Xuan Ming} and Shuji Okada and Hidetosbi Oikawa and Hachiro Nakanishi and Henryk Vogel and David Beljonne and Br{\'e}das, {Jean Luc}",

year = "2000",

month = feb,

doi = "10.1364/JOSAB.17.000256",

language = "English (US)",

volume = "17",

pages = "256--265",

journal = "Journal of the Optical Society of America B: Optical Physics",

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publisher = "The Optical Society",

number = "2",

}

Clays, K, Wostyn, K, Olbrechts, G, Persoons, A, Watanabe, A, Nogi, K, Duan, XM, Okada, S, Oikawa, H, Nakanishi, H, Vogel, H, Beljonne, D & Brédas, JL 2000, 'Fourier analysis of the femtosecond hyper-Rayleigh scattering signal from ionic fluorescent hemicyanine dyes', Journal of the Optical Society of America B: Optical Physics, vol. 17, no. 2, pp. 256-265. https://doi.org/10.1364/JOSAB.17.000256

TY - JOUR

T1 - Fourier analysis of the femtosecond hyper-Rayleigh scattering signal from ionic fluorescent hemicyanine dyes

AU - Clays, Koen

AU - Wostyn, Kurt

AU - Olbrechts, Geert

AU - Persoons, André

AU - Watanabe, Akira

AU - Nogi, Kyoko

AU - Duan, Xuan Ming

AU - Okada, Shuji

AU - Oikawa, Hidetosbi

AU - Nakanishi, Hachiro

AU - Vogel, Henryk

AU - Beljonne, David

AU - Brédas, Jean Luc

PY - 2000/2

Y1 - 2000/2

N2 - 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.

AB - 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.

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U2 - 10.1364/JOSAB.17.000256

DO - 10.1364/JOSAB.17.000256

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VL - 17

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EP - 265

JO - Journal of the Optical Society of America B: Optical Physics

JF - Journal of the Optical Society of America B: Optical Physics

IS - 2

ER -

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

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