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We report three structurally related single ion Dy compounds using the pentadentate ligand 2,6‐bis(( E )‐1‐(2‐(pyridin‐2‐yl)‐hydrazineylidene)ethyl)pyridine (H 2 dapp) [Dy(H 2 dapp)(NO 3 ) 2 ]NO 3  ( 1 ), [Dy(H 2 dapp)(OAc) 2 ]Cl ( 2 ) and [Dy(H 2 dapp)(NO 3 ) 2 ]Cl 0.92 (NO 3 ) 0.08  ( 3 ). The (H 2 dapp) occupies a helical twisted pentagonal equatorial arrangement with two anionic ligands in the axial positions. Further influence on the electronic and magnetic structure is provided by a closely associated counterion interacting with the central N−H group of the (H 2 dapp). The slow relaxation of the magnetisation shows that the anionic acetates give the greatest slowing down of the magnetisation reversal. Further influence on the relaxation properties of compounds 1  and  2  is the presence of short nitrate‐nitrate intermolecular ligand contact opening further lattice relaxation pathways.

Terminal Ligand and Packing Effects on Slow Relaxation in an Isostructural Set of [Dy(H 2 dapp)X 2 ] + Single Molecule Magnets **