Synthetic, Structural and Supramolecular Features of a New Dithiocyanato-κ-N, κ-S-Copper(II) Complex: Insights Through Computational Studies

A new heterocyclic ligand, L [4-(1-methylimidazole)-2,6-di(pyrazinyl)pyridine] has been synthesized and characterized by adequate spectroscopic methods. The title ligand ( L ) was then utilized for synthesizing a new complex, namely, [Cu( L )(NCS)(SCN)]·H 2 O (complex 1 ) and crystallographically characterised by single-crystal X-ray analysis. In the solid state, the complex unit is stabilized through various hydrogen bonding interactions along with π···π stacking and lone pair···π interactions that lead the molecules to generate diverse supramolecular architectures. Interestingly, the complex exhibits weak S···S interaction which has significant contribution in the solid state crystal packing. All the intermolecular interactions that are involved within the structure are quantified through Hirshfeld surface analyses and confirmed by Bader’s theory of ‘atoms-in-molecules’ (AIM). Finally, an interaction energy analysis was carried out to study the interactions between pairs of molecules. Graphical Abstract The present article reports the synthesis, structural elucidation mentioning the role of supramolecular interactions (π···π stacking, lone pair···π and S···S interactions) and theoretical rationalization [quantified through Hirshfeld surface analyses and confirmed by Bader’s theory of ‘atoms-in-molecules’ (AIM)] of a new dithiocyanato-κ-N, κ-S-copper (II) complex derived from heterocyclic ligand, 4-(1-methylimidazole)-2,6-di(pyrazinyl)pyridine.