A new experimental method for observing chromophore relaxation dynamics in nonlinear optical polymer systems is described. The method is similar to dielectric relaxation measurements, which probe the linear susceptibility χ⁽¹⁾, but this new method is chromophore selective and probes the nonlinear susceptibility χ⁽²⁾ in the frequency domain, monitoring second-harmonic generation during the application of a strong ac electric field. The out-of-phase component of χ⁽²⁾ exhibits behavior similar to that of the loss component in dielectric relaxation and is shown to be unaffected by electric-field-induced third-order effects. The relation to dielectric relaxation is discussed, and stretched exponential parameters are extracted for a Disperse-Red-1/poly(methyl methacrylate) guest–host system.

© 1998 Optical Society of America

[Optical Society of America ]

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