A rare disk-like single-molecule magnet (SMM) exclusively bridged by end-on azides with a spin ground state of S = 14 was prepared by the reaction of a divalent FeII precursor with Me3SiN3 under basic conditions. AC magnetic susceptibility studies revealed unusual, "Janus"-faced SMM behavior for the dried and pristine forms of the compound attributed to solvation/de-solvation effects of the coordinated MeCN ligands which leads to alterations in the crystal field and symmetry of the metal ions. DFT calculations confirmed the ferromagnetic nature of the interactions between the FeII spin carriers with the zero-field splitting parameters D = -0.2323 cm-1 and E/D = 0.027. The results have important implications for the future study of single-molecule magnets incorporating volatile solvent molecules in the first coordination sphere of the metal ions and their effect on the relaxation dynamics.
