Abstract
Femtosecond hyper-Rayleigh scattering has been used to probe the spatial orientational fluctuations between nonlinear optical chromophores as dopants in spincoated polymer films. The fluctuation in the second-order incoherently scattered light intensity upon translating the sample is indicative of the degree of spatial correlation between the chromophores. The decay of the autocorrelation function of this fluctuating signal is characterized by a spatial correlation length. Electric-field poling of chromophores is shown to increase this length. The temporal characteristics of this correlation length have been studied and compared with relaxation times, obtained with coherent second-harmonic generation. This correlation length decays much faster than the second-harmonic intensity. The difference in relaxation time between the incoherent and the coherent process is explained by translational diffusion of free volume over the wavelength and over the coherence length, respectively.
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