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Herein we report air-stable Dy(iii) and Er(iii) single-ion magnets (SIMs) with pseudo- D  5h symmetry, synthesized from a sterically encumbered phosphonamide,  t  BuPO(NH i Pr) 2 , where the Dy(iii)-SIM exhibits a magnetization blocking ( T  B ) up to 12 K, defined from the maxima of the zero-field cooled magnetization curve, with an anisotropy barrier ( U  eff ) as high as 735.4 K. The Dy(iii)-SIM exhibits a magnetic hysteresis up to 12 K (30 K) with a large coercivity of ∼0.9 T (∼1.5 T) at a sweep rate of ∼0.0018 T s -1 (0.02 T s -1 ). These high values combined with persistent stability under ambient conditions, render this system as one of the best-characterized SIMs. Ab initio calculations have been used to establish the connection between the higher-order symmetry of the molecule and the quenching of quantum tunnelling of magnetization (QTM) effects. The relaxation of magnetization is observed via the second excited Kramers doublet owing to pseudo-high-order symmetry, which quenches the QTM. This study highlights fine-tuning of symmetry around the lanthanide ion to obtain new-generation SIMs and offers further scope for pushing the limits of U  eff and T  B using this approach.

An air-stable Dy(iii) single-ion magnet with high anisotropy barrier and blocking temperature