Abstract
Abstract Third harmonic generation has been observeb in samples of oriented, fully dense polyacetylene. A theoretical treatment is developed to relate the third harmonic intensity of a thick, absorbing film to its third order nonlinear optical susceptibility, χ(3). A value of χ(3) in excess of 10-8 esu parallel with the polymer chains is inferred from third harmonic intensity measurements. This exceptionally high value of the electronic χ(3) is believed to be the highest ever reported for an organic polymer, an order of magnitude higher than that of polydiacetylene toluene sulphonate.
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