Abstract
The large nonresonant third order optical nonlinearities and fast response times of conjugated polymers make them attractive materials for nonlinear optics. The X(3) spectrum of polyacetylene and polydiacetylenes show similar structure, with magnitudes that agree with calculations of X(3) for the infinite polyene, as well as from the extrapolation of the calculated hyperpolarizabilities of finite polyenes. Of the conjugated polymers, the polydiacetylenes offer the best combination of physical properties since they can be obtained as large single crystals, thin crystalline films, Langmuir-Blodgett multilayers or as spun thin films. Unfortunately, all the conjugated polymers show some sensitivity to oxygen, though single crystals of polydiacetylenes are robust.
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