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

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 compounds1 and 2 is the presence of short nitrate‐nitrate intermolecular ligand contact opening further lattice relaxation pathways.