Abstract
A series of new candidates as nonlinear optical materials, tetra-nuclear heterobimetallic clusters [MOS 3M 3′Y(PPh 3) 3] (M = Mo, M′ = Ag, Y = Br 1; M = W, M′ = Ag, Y = I 2; M = Mo, M′ = Cu, Y = I 3; M = W, M′ = Cu, Y = I 4), have been synthesized by newly developed ligand-redistribution reaction for third-order nonlinear optical (NLO) studies. Single-crystal X-ray diffraction shows that clusters [MoX(μ 3-S) 3(μ 3-Br)(AgPPh 3) 3] 1 and [WX(μ 3-S) 3(μ 3-I)(CuPPh 3) 3] 4 (X = O 0.5S 0.5 1, O 4) adopt an isomorphous neutral cubane-like skeleton. Their optical nonlinearities were measured by Z-scan technique with an 8 ns pulsed laser at 532 nm. These clusters were found to exhibit effective nonlinear absorption, self-focusing effects and large optical limiting capabilities. The effective NLO susceptibilities χ (3) and the corresponding second-order hyperpolarizabilities γ of these clusters are also reported. The influence of cluster composition on NLO properties has been discussed accordingly.
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