Long-wavelength first hyperpolarizability measurements by hyper-Rayleigh scattering.

A hyper-Rayleigh scattering (HRS) system based on an optical parametric power oscillator is described. The first hyperpolarizability, beta, of Crystal Violet dye was measured at 1450 and 1500 nm. The resonance-free beta value, beta(0), for this octupole was found to be comparable with that of the dipolar dye Disperse Red 1 but with the nonlinearity-transparency trade-off worse for the octupole. The discrepancy in beta(0) with that reported previously is explained in terms of resonance and the adequacy of the octupolar three-state model. The possibility of dye aggregation by solvent-dependent HRS is investigated.

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