The authors report the effect of the structure of new synthesized photo-responsive azo dyes, based on N-benzyl-N-ethyl-aniline on their optical and nonlinear optical properties, when doped in polymer and liquid crystal (LC) hosts. Anisotropic response of dyes doped with polymer polymethyl methacrylate is studied using photo-induced birefringence experiment and the optical nonlinearity of dyes doped in LC 5CB is measured using z-scan technique. A correlation is established between dipole moment and optical/nonlinear optical response, which makes it possible to develop molecular design strategies to create structures with suitable anisotropic response and nonlinearity in various host systems for different applications. It is also shown how very little change in the structure of the dye may cause severe changes in the dipole moment and its nonlinear response. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013
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