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In this work, the second- and third-order nonlinear optical response of spin-deposited thin films of three different push-pull side chain azobenzene polymers is investigated by the second- and third-harmonic Maker fringes techniques using 30 ps laser pulses at a fundamental wavelength of 1064 nm. Measurements were carried out before and after aligning the chromophores by corona poling of the films, while different polarization configurations have been utilized. Strong dependence of the response upon the structure of the systems has been found, which is related to the different charge transfer within the molecules. The reported findings are compared with already published results.

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We investigated the optical properties of heterocyclic azo dyes with different side groups prepared: as powders, in PMMA matrix, and side-chain polymers. We characterized the nonlinear optical effects of these compounds by Z-scan and all-optical poling techniques and supported these experiments with theoretical modeling. It was found that these materials show strong two-photon absorption cross sections exceeding 20 GM, which is 1 order of magnitude stronger than that of similar materials (azobenzene and p-amino­azobenzene). Our study reveals the dominant role of the side-chain system over the guest–host one and stresses the importance of the substituent in the efficiency of the poling process.

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