A distinct magnetic anisotropy enhancement in mononuclear dysprosium-sulfur complexes by controlling the Dy-ligand bond length.

In a field-induced single-ion magnet [(dtc)3Dy(phen)] (dtc(-) = diethyldithiocarbamate anion), replacing two of the S-based dtc(-) ligands with O-based dbm(-) ligands (dbm(-) = dibenzoylmethanoate anion) leads to a significant enhancement of magnetic anisotropy, yielding a rarely reported sulfur-ligated lanthanide-based single-ion magnet [(dbm)2Dy(dtc)(phen)]. Ab initio calculations reveal that the gz value of [(dbm)2Dy(dtc)(phen)] is much larger than that of [(dtc)3Dy(phen)], consistent with the experimental results.