A study was conducted to demonstrate the synthesis, processing, linear, and nonlinear optical characterization of substituted polyacetylenes obtained, using ROMP of non-substituted cyclootatetraene (R-COT) monomers. It was demonstrated that that better optical quality of a 200 μm thick poly(n-butyl-COT) film allowed for DFWM image correlation under off-resonant excitation to be preformed with improved diffraction efficiency relative to that obtained, using the diester polyacetylene derivative. It was demonstrated that the process resulted in producing diffracted signals that were strong enough to be captured with a standard VIDICON detector. Polymerization of n-butyl- and sec-butyl-substituted COT monomers, with metal alklyiidene initiators were examined under various conditions, to develop a ROMP-based method for the formation of thick, optical-quality films of polyacetylenes.
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