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Alternation and saturation effects in the chain-length dependences of the third-order hyperpolarizabilities of cyanines

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Abstract

The chain-length dependences of static third-order hyperpolarizabilities γSTAT of the homologous series of thiacyanines, of their meso-nitrogen-substituted derivatives, and of simple bis(dimethylamino)methine dyes are determined from nondegenerate four-wave mixing dispersion curves. We determined nearly the same very rapid increase of γSTAT with growing numbers of π electrons of the chain (γSTAT-N8±2) for both the thiacyanine and the bis(dimethylamino)methine series, an alternating influence of meso-nitrogen substitution for even and for odd double bonds of the chain, and a saturation of the hyperpolarizability for the longest thiacyanine (thiatricarbocyanine). We discuss our results, taking into account semiempirical quantum chemical calculations.

© 1998 Optical Society of America

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