The standard electric-field-induced second-harmonic (EFISH) technique for measurement of the first hyperpolarizability of nonlinear optical molecules is limited by the fact that the second hyperpolarizability also contributes to the second-harmonic signal from which is deduced. We present a modified time-resolved EFISH in which the first and the second hyperpolarizabilities can be determined separately and accurately in the same experiment. We studied para-nitro aniline dissolved in a highly viscous solvent, glycerol, under conditions whereby the electric field was applied faster than the characteristic time for molecular rotation. This technique enabled the contribution to the signal to be resolved separately from the contribution. The results confirm that for this molecule contributes only of the total EFISH hyperpolarizability.
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