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25 February 1993 Quadratic electroabsorption studies of molecular motion in dye-doped polymers
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This paper reports on quadratic electroabsorption studies of thin-film solid solutions of squarylium dye molecules in poly(methylmethacrylate) polymer with the aim of understanding the role of electronic and reorientational mechanisms in the third-order nonlinear-optical susceptibility. We present a generalized theory of the quadratic electrooptic response that includes both electronic mechanisms and molecular reorientation and show that the ratio of two independent third-order susceptibility tensor components, namely (chi) (3)3333/(chi) (3)1133, determines the relative contribution of each mechanism. Based on these theoretical results, we have designed and built an experiment that determines this ratio as a function of temperature and wavelength. Results show that at room temperature and near the first electronic transition wavelength, the response is dominated by the electronic mechanism, and that the reorientational contribution dominates when the sample is heated above its glass transition temperature. Furthermore, results show that, off-resonance, the sign of the imaginary part of the third-order susceptibility is positive. Quadratic electroabsorption is thus shown to be a versatile tool for measuring the imaginary part of the third-order nonlinear-optical susceptibility which yields information about the interaction of polymer and dopant molecule.
© (1993) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.
Constantina Poga, Mark G. Kuzyk, and Carl W. Dirk "Quadratic electroabsorption studies of molecular motion in dye-doped polymers", Proc. SPIE 1775, Nonlinear Optical Properties of Organic Materials V, (25 February 1993);


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