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

Chemical Science, ISSN: 2041-6539, Vol: 7, Issue: 8, Page: 5181-5191
2016
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Herein we report air-stable Dy(iii) and Er(iii) single-ion magnets (SIMs) with pseudo-D symmetry, synthesized from a sterically encumbered phosphonamide, BuPO(NHPr), where the Dy(iii)-SIM exhibits a magnetization blocking (T) up to 12 K, defined from the maxima of the zero-field cooled magnetization curve, with an anisotropy barrier (U) 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 (0.02 T s). 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 and T using this approach.

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