This account concerns the synthesis, structures and magnetism of cyanide-bridged bimetallic network compounds. The study aims at the development of molecular-based magnetic materials. Different network structures, from one-dimensional to three-dimensional, are synthesized by the reaction of [M(CN)6]n- with a cationic constituent such as [Ni(diamine)2]2+, [Ni(triamine)]2+, [Mn(salen)]+, [Mn(en)]2+, etc., in the absence or presence of an appropriate counter ion. Magnetostructural studies for those bimetallic compounds have clarified fundamental factors contributing to magnetic ordering in bulk, magnetic nature (ferromagnetism or metamagnetism) and magnetic phase-transition temperature (Tc). The strategies for gaining high Tc magnetic material and modulating magnetic nature by a change in network structure are described.
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