Construction of Nitronyl Nitroxide‐Based 3d–4f Clusters: Structure and Magnetism

Three unprecedented nitronyl nitroxide radical‐bridged 3d–4f clusters, [Ln 2 Cu 2 (hfac) 10 (NIT‐3py) 2 (H 2 O) 2 ](Ln III =Y, Gd, Dy), have been obtained from the self‐assembly of Ln(hfac) 3 , Cu(hfac) 2 , and the radical ligand. The Dy complex shows a slow relaxation of magnetization, representing the first nitronyl nitroxide radical‐based 3d–4f cluster with single‐molecule magnet behavior.