Nickel-bisdithiolate complexes with a ferrocene-containing 2nd order nonlinear optical chromophore as a cation, (FcCH=CHPyMe)[NiL 2 ] where L=dmit (1a), dddt (1b) and debt (1c) were synthesized by the cation exchange reaction. In the X-ray crystal structure of complex (1a), no intrastack but interstack S…S interactions less than 3.7 Å are observed. This complex was revealed to be an insulator at room temperature. However, (FcCH=CHPyMe) x [Ni(dmit) 2 ] (0<x<1) (3) needle grown in an H-type electrochemical cell shows semiconductor behavior (E a =106 meV) over the temperature range measured (30∼300 K) with σ RT =1 Ω −1 cm −1. The electronic transition at UV-vis-NIR region was measured for the nickel complexes and discussed.
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