Two new cyano-bridged mixed-valence {Fe III 2 (μ-CN) 4 Fe II 2 } clusters, {[(Tp)Fe III. Complexes 1 and 2•5MeOH exhibit gradual thermally induced two-step spin-crossover behavior (SCO) at two Fe II metal centers, and the transformation of high-spin (HS) to low-spin (LS) Fe II ions with temperature was confirmed by a combination of X-ray crystallography, variabletemperature Fourier transform infrared, variable-temperature magnetic susceptibility, and 57 Fe Mossbauer spectroscopy. Moreover, complexes 1• MeCN•Et 2 O and 1 exhibit a reversible single-crystal-to-single-crystal transformation, and complex 1 undergoes two-step SCO behavior with T 1/2 = 178 and 93 K accompanied by symmetry breaking in the structure.

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Cyano-bridged mixed-valence {Fe6} hexanuclear complexes {[Tp4-MeFeII(CN)3]2[FeIII(Tpa)]2[FeIII(OR)(Tpa)]2}·6ClO4·S {Tp4-Me = tri(4-methyl-pyrazol-1-yl)borate, Tpa = Tris(2-pyridylmethyl)amine; R = -CH3 S = 8MeOH 1, R = -C2H5 S = 6EtOH 2 } have been obtained...