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A series of mononuclear Dy III complexes with the general formula [DyLz 2 (salicylaldehyde) 2 ]·X·solvent (Lz = 6-pyridin-2-yl[1,3,5]triazine-2,4-diamine; X = OH - (1·OH), Cl - (2·Cl), Br - (3·Br)) have been synthesized using mixed salicylaldehyde/pyridinyl-triazine ligands and discriminative counteranions. The Dy III ion in these three complexes resides in a similar D 4d coordination geometry with counteranions perturbing the coordination environment and bond lengths and angles in the lattice. Magnetostructural studies reveal that the asymmetric distribution of salicylaldehyde/pyridinyl-triazine ligands and the presence of discriminative counteranions result in the coexistence of large anisotropy and quantum tunneling of magnetization. The magnetic anisotropy is dominated by the axial ligand field with short Dy-O sali distances and large ∠O sali -Dy-O sali angles, while the quantum tunneling relaxation is probably dictated by the π-π stacking of the Lz ligands, which induces an axial constriction of the coordinating plane. Ab initio calculations substantiate the diversity of the magnetic behaviors in these complexes and highlight the importance of axial ligand field with short Dy-O sali distances, large ∠O sali -Dy-O sali angles and less ligand stacking in these pseudo-D 4d -symmetrical single-molecule magnets.

Axial Ligand Field in D4d Coordination Symmetry: Magnetic Relaxation of Dy SMMs Perturbed by Counteranions

Axial Ligand Field in D_4d Coordination Symmetry: Magnetic Relaxation of Dy SMMs Perturbed by Counteranions