Syntheses, crystal structures, and magnetic properties of Ni(mnt)2-based molecular solids containing substituted isoquinolinium

Two novel ion-pair complexes, [RBzIQl]+[Ni(mnt)2]− (mnt2− = maleonitriledithiolate, [RBzIQl]+ = 4-R-benzylisoquinolinium; R = H (1), Cl (2)) have been characterized structurally and magnetically. The anions and cations in 1 form 1D column of alternating between cations and anions, while those of 2 stack into well-segregated columns and the Ni(III) ions form a 1D uniform zigzag chain. The former shows antiferromagnetic coupling behavior, and the latter exhibits antiferromagnetic interaction in the high-temperature phase (HT) and spin gap in the low-temperature phase (LT).