Abstract

Abstract Reaction between the dimeric [Mn2(saltmen)2(H2O)2]2+ cations (with saltmen = N,N′-(1,1,2,2-tetramethylethylene)bis(salicylideneiminato) dianion) and [Cr(CN)6]3− anions results in the isolation of a 2D layered complex, [{Mn(saltmen)}4Cr(CN)6]ClO4 (1), whose crystal structure has been determined and presents pentameric cyanido-bridged CrMn4 units assembled into extended layers through saltmen phenoxo Mn–Mn bridges. Detailed magnetic measurements and their analysis show that the layers have a ferrimagnetic organization with antiferromagnetic exchange coupling (J/kB = −7(1) K) between Mn(III) and Cr(III) ions through cyanide bridges and ferromagnetic interaction between Mn(III) ions through phenoxo bridges. Compound 1 displays a glassy ferrimagnetic ordering with TC = 5 K. Magneto-structural discussions for 1 and three similar 2D systems are developed that explain the antiferromagnetic coupling observed in the cyanido-bridged Mn(III)–Cr(III) cases.

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