“…Therefore, it is meaningful for the design and preparation of new counter-cations for adjust the overlap patterns of [Ni(mnt) 2 ] − anions in order to build a relationship between the intermolecular and its function. In recent years, we have systemically investigated the influence of derivatives of 2 or 4-substituted benzyl triphenylphosphonium ([2RBzTPP] + and [4RBzTPP] + , R = H, F, Cl, Br, NO 2 ) as multifunctional counter-cation of upon the overlapping mode of the neighboring [Ni(mnt) 2 ] − anion and the magnetic coupling of the molecular metals, which generally involve aromatic · · · stacking, weak coordinative forces, short-range interactions and hydrogen bonds [16][17][18][19][20]. With a view to extending our study in this field, we have obtained two molecular solids containing disubstituted benzyl triphenylphosphonium cations, [2F4BrBzTPP] [Ni(mnt) 2 [21,22].…”