Rational Design and Construction of Polymers with Large Second-Order Optical Nonlinearities. Synthetic Strategies for Enhanced Chromophore Number Densities and Frequency Doubling Temporal Stabilities

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Abstract
The performance characteristics of poled polymeric second harmonic generation materials are crucially dependent upon achieving high number densities of constituent chromophore entities and on maintaining poling-induced microstructural acentricity. This article reviews recent progress toward these goals. Systems discussed include chromophore-functionalized polyphenylene ether macromolecules with second harmonic coefficients (d33) as high as 65 × 10−9 esu, Tg = 173°C, and with superior temporal stability of poling-induced chromophore orientation. Also discussed are strategies for simultaneously poling and diepoxide cross-linking chromophore-functionalized poly(p-hydroxystyrene). The result is a significant improvement in the temporal stability of chromophore orientation. Finally, two approaches to chromophore immobilization are presented which involve highly cross-linkable epoxy matrices. In the first, chromophore molecules are embedded in a matrix which is simultaneously poled and thermally cured. In the second, a functionalized high-β chromophore is synthesized for use as a cross-linking matrix component.

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