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Herein, we reported the synthesis of copper(I) thiocyanate complexes with ortho-pyridinyl carbohydrazones containing a thiophene (L1) or a furyl ring (L2) as a mixture of two different crystals for each compound, linkage isomers of C1N, [Cu(NCS)(L1)PPh3] and C1S, [Cu(SCN)(L1)PPh3], for L1, whereas monomeric and polymeric structures C2N, [Cu(NCS)(L2)PPh3], and C2P, [–(NCS)Cu(L2)–]n, for L2. Crystallographic information and theoretical calculations, mainly noncovalent interaction reduced density gradient (NCI-RDG) analyses, were pursued to generate a profound understanding of the structure-directing interactions in these complexes. The supramolecular assemblies are first driven by cooperative π⋯π interactions and hydrogen bonds followed by CH⋯π, S⋯S and S⋯π linkages. In the case of the linkage isomers, intermolecular interactions may have a significant role in the formation of the less stable S-bound isomer C1S.

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Investigation of structure-directing interactions within copper<scp>(i)</scp>thiocyanate complexes through X-ray analyses and non-covalent interaction (NCI) theoretical approach

Investigation of structure-directing interactions within copper(i)thiocyanate complexes through X-ray analyses and non-covalent interaction (NCI) theoretical approach