Abstract
Two new salts of bis(2-thioxo-1, 3-dithiole-4, 5-dithiolato) nickelate monoanion with 4-amino-1-heptylpyridinium (1) and 4-amino-1-nonylpyridinium (2) were prepared and characterized. Two isostructural salts with anion/cation=1:1 crystallize in space group P-1 with similar cell parameters and packing structures. The anions and cations form alternating layered arrangements, which are connected via charge-assisted S⋯H H-bonds. Within an anion layered alignment, the magnetic exchange is transmitted between the neighboring anions via three types of pathways (face-to-face π–π stack, lateral-to-lateral and head-to-tail S⋯S contacts), where the stronger antiferromagnetic coupling occurs between the face-to-face stacked anions, owing to π-type magnetic orbitals efficiently overlapped, than others and dominates the magnetic nature of 1 and 2. The dielectric and conducting properties were also investigated for two salts in the temperature range of 175–375K.
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