Tetraalkylammonium cyanides react with Mn(II) salts under anerobic conditions to form extended 2- and 3-D structured percyanomanganates(II) of AmMnIIn(CN)m+2n composition, e.g. AMnII3(CN)7, A2MnII3(CN)8,A2MnII5(CN)12, A3MnII5(CN)13, and A2MnII[MnII(CN)6]. The high-spin Mn(II) sites lack sufficient electrostatic cation+-NC stabilization and only form 4- and 5-coordinated Mn sites within a flexible, extended framework around the cation; hence, the size, shape, and charge of the cation dictate the unprecedented stoichiometry and unpredictable cation adaptive structures. In all cases, antiferromagnetic coupling between adjacent MnIIsites leads to ferrimagnetic ordering, but in some cases antiferromagnetic coupling of the ferrimagnetic layers are compensated and synthetic antiferromagnets are observed

Ferri- and antiferromagnetically ordered, cation adaptive structures based upon tetraalkylammonium percyanomanganate(II)

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