The mononuclear complex [Ni(HOphen)(OSO3)(H2O)3]·5H2O (HOphen = 1, 10‐phenanthrolin‐2‐ol) was prepared and its single structure was determined by X‐ray crystallography. In this complex, the NiII ion has a distorted octahedral arrangement. Crystal structure analysis shows that two kinds of π–π stacking interactions and C–H···O short contact intermolecular interactions exist among the adjacent complexes. Fitting to the variable‐temperature magnetic susceptibility data gave the magnetic coupling constant, 2J = –0.98 cm–1. Theoretical calculations, based on density functional theory (DFT) coupling with the broken‐symmetry approach (BS), revealed that the π–π stacking magnetic coupling pathways resulted in weak ferromagnetic interactions with 2J = 4.86 cm–1 and 2J = 4.16 cm–1, respectively, for the adjacent NiII ions with separations of 8.568(19) Å and 8.749(32) Å, respectively; whereas the magnetic coupling pathway of the C–H···O short contact intermolecular interaction led to a weak antiferromagnetic interaction with 2J = –17.62 cm–1 for the adjacent NiII ions with a separation of 10.291(26) Å. The ferromagnetic coupling sign can be explained by the McConnell I spin‐polarization mechanism.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.