Single-molecule magnets (SMMs) that can be trapped in one of the bistable magnetic states separated by an energy barrier are among the most promising candidates for high-density information storage, quantum processing, and spintronics. To date, a considerable series of achievements have been made. However, the presence of fast quantum tunnelling of magnetization (QTM) in most SMMs, especially in single-ion magnets (SIMs), provides a rapid relaxation route and often sets up a limit for the relaxation time. Here, we pursue the pentagonal bipyramidal symmetry to suppress the QTM and present pentagonal bipyramidal Dy(III) SIMs [Dy(CyPO)(HO)]Cl·(CyPO)·HO·EtOH (1) and [Dy(CyPO)(HO)]Br·2(CyPO)·2HO·2EtOH (2), (CyPO = tricyclohexyl phosphine oxide). Magnetic characterizations reveal their fascinating SMM properties with high energy barriers as 472(7) K for 1 and 543(2) K for 2, along with a record magnetic hysteresis temperature up to 20 K for 2. These results, combined with the ab initio calculations, offer an illuminating insight into the vast possibility and potential of what the symmetry rules can achieve in molecular magnetism.
陈龑骢 刘俊良 Liviu Ungur Liu Jiang Li Quan-Wen Wang Long-Fei Zhaoping Ni Liviu Chibotaru 陈小明 童明良
Journal of the American Chemical Society