Binuclear Cluster-to-Cluster-Based Supramolecular Compounds: Design, Assembly, and Enhanced Third-Order Nonlinear Optical Performances of {[Et<sub>4</sub>N]<sub>2</sub>[MoOS<sub>3</sub>Cu<sub>2</sub>(μ-CN)]<sub>2</sub>·2aniline}<sub><i>n</i></sub> and {[Et<sub>4</sub>N]<sub>4</sub>[MoOS<sub>3</sub>
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Reaction of a cluster precursor [Et4N]2[MoOS3(CuCN)] (1) with equimolar [Cu(MeCN)4](PF6) in MeCN/aniline gave rise to an interesting polymeric cluster {[Et4N]2[MoOS3Cu2(μ-CN)]2·2aniline}n (2), while treatment of 1 in MeCN with 2 equiv of CuCN and KCN in H2O afforded the other polymeric cluster {[Et4N]4[MoOS3Cu3CN(μ′-CN)]2(μ-CN)2}n (3). Generated by addition of one or two Cu+ onto the [MoOS3Cu] cluster core in 1, the butterfly shaped [MoOS3Cu2] fragment in 2 or the incomplete cubanelike [MoOS3Cu3] fragment in 3 was dimerized into a prismatic [MoOS3Cu2]2 cage core or a double incomplete cubanelike [MoOS3Cu3]2 core. These two expanded cores serve as a unique planar 4-connecting node (2) or a rare chairlike 4-connecting node (3) to link equivalent nodes via cyanide bridges, forming two kinds of different 2D (4,4) networks. The third-order nonlinear optical (NLO) properties of 1−3 in DMF were also investigated.
