Abstract
Since the introduction of Hyper-Rayleigh scattering (HRS) as a measurement technique for the first hyperpolarizability of molecules in solution,1 the importance of fluctuations was realized.2 For isotropic solutions, a combination of the spatial and temporal orientational fluctuations causes the instantaneous and local deviation from macroscopic centrosymmetry, necessary to observe a second-order signal. The fluctuations in the spatial orientational distribution function of nonlinear optical chromophores cause an HRS signal that fluctuates as a function of position in solid samples. The correlation length, characterizing the decay of the autocorrelation function of this fluctuating signal, indicates the degree of spatial correlation between these chromophores. The development of femtosecond HRS was instrumental for the study of orientational correlations.3
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