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We have reported previously that metal poly-ynes have large thirdorder optical susceptibilities. Based on the four-wave mixing studies reported here, we conclude that strong two-photon absorptions in metal poly-ynes contribute significantly to the observed third-order nonlinearities of these materials. Hyperpolarizability/r.u. increases only slightly with chain length for tetrahydrofuran solutions of the metal poly-ynes. The possible influence of conformers on this behavior is discussed.

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