3D network structure and spin gap behavior in two new molecular magnets based on bis(maleonitriledithiolato)nickelate monoanion

Two new molecular magnets, [DiBrBzPy][Ni(mnt)2]− (1) and [DiBrBzIQl][Ni(mnt)2] (2) ([DiBrBzPy]+ = 1-(3′,5′-dibromobenzyl)pyridinium, [DiBrBzIQl]+ = 1-(3′,5′-dibromobenzyl)isoquinolinium and mnt2− = maleonitriledithiolate), form a 3D network structure through weak Ni⋯N, C⋯N short interactions, π⋯π stacking interactions, and C-H⋯Br, C-H⋯N hydrogen bonds, and exhibit the typical magnetic behavior of a spin gap system.