Second-order nonlinear-optical properties of donor- and acceptor-substituted aromatic compounds

Nonresonant second-order microscopic nonlinear-optical susceptibilities (β) of a series of organic conjugated π-electron molecules were measured, using dc-induced second-harmonicgeneration. This study confirms structure–property relationships that affect β, including the electronic properties of substituents, the length of and type of π-electron system, molecular configuration, and dispersion. A quantity β0, based on a two-level model, is used, allowing trends to be discerned more easily by dividing out the effects of the dispersion of the first excited state. The second-order microscopic susceptibilities of materials based on cyanovinyl-substituted azobenzenes and stilbenes are found to be large. Details of the experimental configuration and method are also presented.

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