期刊
CHEMICAL SCIENCE
卷 7, 期 8, 页码 5181-5191出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6sc00279j
关键词
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资金
- DST Nanomission [SR/NM/NS1119/2011]
- SERB, New Delhi [SB/S2/JCB-85/2014]
- IIT-Bombay
- DAE-BRNS for the Outstanding Investigator Award
- SERB [EMR/2014/000247]
- UGC, New Delhi
- IRCC, IIT Bombay
- CSIR
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, (BuPO)-Bu-t((NHPr)-Pr-i) 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 similar to 0.9 T (similar to 1.5 T) at a sweep rate of similar to 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.
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