Abstract
The importance of structural factors like dimensionality and order on the nonlinear optical properties of conjugated polymers are discussed. In the case of polydiacetylene one can obtain monooriented thin films by epitaxy through monomer evaporation under high vacuum and its subsequent polymerization. Optical third harmonic generation measurements confirm the enhanced X(3) susceptibility in polymer chain direction with a very large anisotropy (X ‖ (3) /X ⊥ (3) >140). On the other hand, nonlinear optical techniques turn out to be a useful tool for checking orientation of conjugated polymer chains, even in the case when linear dichroism techniques fail.
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