Dysprosium Single‐Molecule Magnets with Bulky Schiff Base Ligands: Modification of the Slow Relaxation of the Magnetization by Substituent Change

: The synthesis, and magnetic and photoluminescence investigations of two bifunctional dysprosium complexes based on tridentate Schiff base ligands is reported. Magnetic investigations reveal a genuine single-molecule magnet (SMM) behavior, with out-of-phase signals up to 60 K, and tunable emission arising from the Schiff base ligands.