Nonlinear Optics Of Molecular Aggregates

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Abstract
We report a new class of molecules, pyrylium dye aggregates, that possess exceptionally large second-order optical nonlinearity. These dye molecules aggregate spontaneously in a polymer matrix to form a head-to-tail ordered structure. We have observed efficient second harmonic generation in a micron-size thin film containing only 1.5 wt% dye aggregate. This observation suggests the exciting possibility of achieving significant nonlinear optical interaction within one coherence length. Semi-empirical molecular orbital calculations also suggest that these dyes possess large second-order polarizabilities. We suggest that charge-transfer excitons within the aggregates may account for the large observed nonlinearities.© (1987) COPYRIGHT SPIE--The International Society for Optical Engineering. Downloading of the abstract is permitted for personal use only.

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