Modulating Magnetic Performance in DyIII Single Ion Magnets With N5O2 Ligands

ABSTRACT Dy (L Me )(H 2 O)CF 3 SO 3 ·0.25H 2 O ( 1 ·0.25H 2 O), where H 2 L Me is the reported ligand 2,2′‐(((pyridine‐2,6‐diylbis (methylene))bis((pyridin‐2‐ylmethyl)azanediyl))bis (methylene))bis(4‐methylphenol), shows the Dy III ion in an N 5 O 3 environment, with triangular dodecahedral geometry (D 2d symmetry). 1 ·0.25H 2 O is a single ion magnet (SIM) with an energy barrier for spin reversal of 510 K, and open hysteresis loops up to 8 K. The magnetostructural comparison of 1 ·0.25H 2 O with some closely related complexes and with other eight‐coordinated SIMs with high energy barriers (> 300 K) allows to draw some conclusions to enhance the magnetic performance in these nanomagnets with non‐purely axial geometries. Ab initio calculations complement and support the experimental results.