The magnetic relaxation dynamics of low-coordinate Dy(III) and Er(III) complexes, namely three-coordinate ones with an equatorially coordinated triangle geometry and five-coordinate ones with a trigonal bipyramidal geometry, have been exploited for the first time. The three-coordinate Er-based complex is the first equatorially coordinated mononuclear Er-based single-molecule magnet (SMM) corroborating that simple models can effectively direct the design of target SMMs incorporating 4f-elements.
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