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We have measured the third-order susceptibility, X((3)), versus concentration for a number of molybdenum-based metal-organic complexes in solution, using independent degenerate four-wave mixing and Z-scan techniques. Good agreement was obtained between the degenerate four-wave mixing and Z-scan measurements. The variation of X((3)) with concentration yielded the second-order hyperpolarizability gamma. A close correlation was observed between the number of delocalized pi electrons and the magnitude of gamma.

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Nonlinear optical properties of transition metal-phosphine complexes have been measured at 532 nm by degenerate four-wave mixing. Large second-order molecular hyperpolarizabilities, γ, have been found for complexes containing two phosphine ligands. The measured γ values are closely related to the type and coordination geometry of the phosphine ligands, and the γ values vary as the fifth power of the number of substituents with π-electrons structure.