The employment of 1‐((2‐hydroxybenzylidene)amino)‐2,3‐dihydro‐1H‐inden‐2‐ol (H2L) in ZnII and CoII coordination chemistry is reported. Two complexes of compositions [Zn4L4] (1) and [Co4L4] (2) have been synthesized under solvothermal conditions, and fully characterized by X‐ray single crystal diffraction, IR and elemental analysis. They both possess a defect dicubane core. The luminescence studies suggest strong emission for 1 in the solid state at room temperature. Variable temperature (2.0–300 K) magnetic studies for 2 indicate weak ferromagnetic CoII⋅⋅⋅CoII exchange interactions.
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