Electric-field-induced second-harmonic generation experiments on polydiacetylene solutions in dimethylformamide and in chloroform at 1.064 {μ}m fundamental wavelength are presented. The technique allows for the measurements of both modulus and phase of the cubic susceptibility χ⁽³⁾(-2{ω};{ω},{ω},0). Influence of the phase on the measured harmonic intensities is discussed in detail as well as errors which can result when it is neglected. It is found that χ⁽³⁾(-2{ω};{ω},{ω},0) is complex with negative real part. This result is discussed in terms of a two-photon resonance. A small solvatochromic effect is also observed.
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Kajzar et al. (1987) studied this question.
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