Syntheses, Structures, and Magnetic Properties of Two DMTCNQ and DETCNQ Gadolinium Complexes.

Two DMTCNQ (DMTCNQ = 2,5‐dimethyl‐7,7,8,8‐tetracyano‐p‐quinodimethane) and DETCNQ (DETCNQ = 2,5‐diethyl‐7,7,8,8‐tetracyano‐p‐quinodimethane) gadolinium complexes [Gd(DMTCNQ)2(CH3OH)(H2O)6][DMTCNQ]·4H2O (1) and [Gd(DETCNQ)(H2O)7][2DETCNQ] (2) were synthesized by reactions of GdCl3·6H2O with Li(DMTCNQ) or Li(DETCNQ). X‐ray diffraction analysis reveals that complexes 1 and 2 are discrete complexes. The central metal atom in 1 is coordinated by two DMTCNQ ligand radicals whereas that in 2 is coordinated by just one DETCNQ ligand radical. The adjacent molecules are connected by the intermolecular hydrogen bonds to form the two‐dimensional (2D) supramolecular layer structures, which are further packed into a three‐dimensional (3D) supramolecular architecture through the π–π interactions between ligand radicals in 1 and 2. Magnetic investigation indicates that the antiferromagnetic interactions between spin carriers exists in 1 and 2. [ABSTRACT FROM AUTHOR]