Abstract

Main observation and conclusionTwo chelating guanidinate‐based dysprosium(III) complexes, namely the monomeric {(Me3Si)2NC(NiPr)2}2Dy(μ‐Cl)2Li(THF)2 1 and the dimeric [{(Me3Si)2NC(NiPr)2}2Dy(μ‐Cl)]2 2, have been confirmed to be single‐molecule magnets. Moreover, the alteration from 1 to 2 leads to an obvious mitigated quantum tunnelling of magnetization at zero field of the hysteresis loop and much enhanced magnetic relaxation barrier (up to 312 K). 5% dilution with the yttrium(III) analogue for 2 shows no clear change for the hysteresis, indicating the single‐ion nature of the magnetic behavior.

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