In the field of molecular magnetism, the lanthanide-radical (Ln-Rad) method has become one of the most appealing tactics for introducing strong magnetic interactions and has spurred on the booming development of heterospin single-molecule magnets (SMMs). The article is a timely retrospect on the research progress of Ln-Rad heterospin systems and special attention is invested on low dimensional Ln-Rad compounds with SMM behavior, primarily concerning with nitrogen-based radicals, semiquinone and nitroxide radicals. Rational design, molecular structures, magnetic behaviors and magneto-structural correlations are highlighted. Meanwhile, particular attention is focused on the influence of exchange couplings on the dynamic magnetic properties, with the purpose of helping to guide the design of prospective radical-based Ln-SMMs.
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