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Single-molecule magnets (SMMs) exhibiting open hysteresis loops maypotentially apply to molecule-based information processing and storage.However, the capacity to retain magnetic memory is always limited by zero-fieldquantum tunneling of magnetization (QTM). Herein, a well-designed dysprosiummetallacrown SMM, consisting of an endohedral approximate linear F-Dy-F stronganisotropic moiety in a peripheral [15-MCNi-5] metallacrown (MC), is reportedwith the largest reversal barrier of 1060 cm-1 among d-f SMMs. Rectangle-likehysteresis loops are observed with the huge squareness (remanence/saturationmagnetization) up to 97% at 2 K. More importantly, zero-field QTM step isphenomenologically removed by minimizing the dipole coupling and hyperfineinteractions. The results demonstrate for the first time that zero-field QTMstep can be eliminated via manipulating the ligand field and vanishing theexternal magnetic perturbations, which illuminates a promising blueprint fordeveloping high-performance SMMs.

Rectangle-like hysteresis in a Dysprosium Metallacrown Magnet with Linear F-Dy-F Anisotropic Moiety