Abstract
Even-order nonlinear optical processes are forbidden, in the electric-dipole approximation, in centrosymmetric material systems such as an isotropic solution of achiral molecules. However, orientational fluctuations of noncentrosymmetric molecules can break locally the macroscopic centrosymmetry of such solutions and make incoherent nonlinear scattering processes possible. Second-order elastic and inelastic scattering at the second-harmonic frequency of the fundamental laser beam was first observed in 1965 from several materials.1 More recently, elastic scattering at the exact second-harmonic frequency (hyper-Rayleigh scattering) has gained popularity as a routine technique to determine the first hyperpolarizability of organic molecules in solution.2
© 1995 Optical Society of America
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