Abstract

The third-order optical nonlinearities and responses of poly(methylmethacrylate) (PMMA) coating films containing J-like aggregates of athiadicarbocyanine dye, 3,3′-diethyl-2,2′-thiadicarbocyanine iodide(DTDCI), are measured by degenerate four-wave mixing (DFWM) techniqueunder resonant conditions. The temporal profiles of the DFWM signal ofPMMA coating films containing J-like aggregates of DTDCI are found toconsist of three components: i.e., the coherent instantaneous nonlinearresponse (electronic response) and the two slow responses with decaytime constants of about 0.8 ps and about 7.0 ps. The electroniccomponent of the effective third-order nonlinear susceptibility,χ(3)e, of one of the present films is as high as about 2.1×10−8 esu, and the figure of merit of third-order nonlinearity F(F = χ(3)/α) is evaluated to be about 1.9×10−13 esu cmat 850 nm.

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