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Proceedings Paper

Hyper-Rayleigh scattering for symmetry fluctuation spectroscopy
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Paper Abstract

Incoherent second-order nonlinear scattering, or hyper-Rayleigh scattering (HRS) has been evaluated as a new experimental tool for symmetry fluctuation spectroscopy. As such, it is the second-order nonlinear analogue of the linear dynamic light scattering (DLS) of quasi-elastic light scattering (QELS) technique for density fluctuation spectroscopy. High peak power is needed in a short pulse for the second-order nonlinear optical effect to be observed. The periodical structure of the impinging light itself does not impede the measurement for intensity correlation times longer than the pulse-to-pulse period. However, the inherently large spectral bandwidth of femtosecond pulses considerably reduces the amplitude of the autocorrelation function. Reducing the coherence volume to increase this amplitude results in a lower count rate. The low efficiency of the second-order nonlinear light scattering, possible relaxation oscillation in solid-state femtosecond lasers and its quadratic amplification in second-order nonlinear scattering have pronounced influence on the autocorrelation function. Finally, typical relaxation times expected for the dynamics associated with large fluctuations in second-order nonlinearity put a severe limit on the applicability of quasi-elastic nonlinear light scattering for the study of chemical reaction dynamics.

Paper Details

Date Published: 1 November 2002
PDF: 11 pages
Proc. SPIE 4812, Nonlinear Spectroscopy, (1 November 2002); doi: 10.1117/12.451376
Show Author Affiliations
Koen J. Clays, Katholieke Univ. Leuven (Belgium)
Andre P. Persoons, Katholieke Univ. Leuven (Belgium)

Published in SPIE Proceedings Vol. 4812:
Nonlinear Spectroscopy
David L. Andrews, Editor(s)

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