Single-Molecule\nMagnet Behavior in a Tb-Nitronyl Nitroxide\nRadical Network with [Tb<sub>3</sub>(NIT)<sub>2</sub>] Nodes

Two\nrare two-dimensional Ln-radical networks, namely, [{Ln(tfa)<sub>3</sub>}<sub>3</sub>(NIT-4Py)<sub>2</sub>]<sub><i>n</i></sub> [Ln<sup>III</sup> = Gd <b>1</b> and Tb <b>2</b>; tfa<sup>–</sup> = trifluoroacetylacetonato; and NIT-4Py\n= 2-(4-pyridyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide], have\nbeen successfully constructed and characterized. In these complexes,\neach NIT-4Py radical functions as a tridentate ligand to ligate three\nLn ions, creating a 2D network with linear five-spin [Ln<sub>3</sub>(NIT)<sub>2</sub>] nodes. Ferromagnetic Ln-NO interactions govern\nthe characteristic magnetic behavior of a finite spin system. The\nTb complex is shown to exhibit SMM behavior in a zero DC field, with\nan energy barrier for spin flipping of 53 K and hysteretic M-H behavior\nat 2.3 K, with a coercive field <i>H</i><sub>coer</sub> =\n110 Oe. This complex represents the first example of a Ln-nitronyl\nnitroxide SMM-based network.