Abstract

Abstract A cyanide-bridged molecular square, [Co2Fe2(CN)6(tp*)2(dtbbpy)4](PF6)2·2MeOH (1) (tp* = hydrotris(3,5-dimethylpyrazol-1-yl) borate and dtbbpy = 4,4′-di-tert-butyl-2,2′-bipyridine) was prepared by the reaction of (Bu4N)[Fe(CN)3(tp*)] with Co(CF3SO3)2·6H2O and dtbbpy in methanol. Variable temperature X-ray structural analyses, magnetic and spectroscopic data revealed that 1 exhibited novel thermal two-stepped spin transitions induced by intramolecular electron transfers.

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