Journal of Chemical Physics, Vol.113, No.21, 9706-9713, 2000
Dynamic light scattering with femtosecond laser pulses: Potential and limitations toward quasielastic nonlinear light scattering
We have implemented dynamic linear and second-order nonlinear light scattering with femtosecond laser pulses. 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 quasielastic nonlinear light scattering for the study of chemical reaction dynamics.