Polymeric materials with large nonlinear optical (NLO) coefficients are of interest for their potential use in electrooptic applications.1™3 The chromophores in the polymer matrix are oriented in a noncentrosymmetric fashion by poling for bulk second-order NLO properties.4™7 A major shortcoming of poled polymeric materials is the lack of long-term stability of the NLO properties. Promising schemes to overcome this problem include the incorporation of the aligned chromophores into crosslinked network structures or polymers with rigid backbones.7™11

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