Abstract
Third-order nonlinear optical susceptibilities χ(3)(−3ω; ω, ω, ω) have been measured by third-harmonic generation for thin films of a series of polysilane polymers and copolymers and polycarbosilanes with different alkyl and aryl side groups. χ(3)(−3ω; ω, ω, ω) values for all the polymers studied were found to be in the range 0.3 × 10−12–4.5 × 10−12 esu. Factors affecting the magnitude of χ(3), including the nature of the substituents, Si sequence length, polymer conformation, and film preparation, are discussed.
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