Abstract

The standard electric-field-induced second-harmonic (EFISH) technique for measurement of the first hyperpolarizability $\left(\beta \right)$ of nonlinear optical molecules is limited by the fact that the second hyperpolarizability $\left(\gamma \right)$ also contributes to the second-harmonic signal from which $\beta$ 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 $\gamma$ contribution to the signal to be resolved separately from the $\beta$ contribution. The results confirm that for this molecule $\gamma$ contributes only $\sim 10\%$ of the total EFISH hyperpolarizability.

© 2002 Optical Society of America

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