Abstract
The chain-length dependences of static third-order hyperpolarizabilities 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 with growing numbers of π electrons of the chain 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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