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Published online by Cambridge University Press: 21 February 2011
Third-order optical nonlinearity in organic materials has generally been sought from molecules and polymers having extended i-electron delocalization in conjugated bonding schemes. In an alternative approach, we have investigated the third-order optical response of a polymeric composite containing charge transfer complexes in which the nonlinearity originates from intermolecular electron delocalization between π-electron clouds in charge transfer stacks. The material, which is composed of a polymer having electrondonating pendant side groups that complex with dopant electron-acceptor molecules, has been processed into an optically clear thin film. Nonlinear characterization of the film by means of third-harmonic generation suggests enhancement of the third-order response arising from charge transfer interactions.