Heterometallacrowns as high-spin molecules
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Abstract
The achieved results of the two here described sub-projects of heterometallic and heterovalent cobalt metallacoronates provide significant contributions to the areas of metallacrown chemistry as well as single-molecule magnetism based on virtually magnetically isolated transition metal ions and have simultaneously proven the high capability of both new developed strategies to exploit the distinguished features of 12-MC-4 transition metal complexes for the research on single-molecule magnets.
The first 3d heterometallic 12-MC-4 metallacoronate Cu(II)(DMF)2Cl2[12-MCFe(III)N(Shi)-4](DMF)4 has been designed according to a novel magnetic director approach and synthetically realized. Causing a high-spin ground state of approximately S = 11/2, the new developed concept accomplishes its intension to overcome the common mutual cancelation of the spins in 12-MC-4 complexes by superior radial antiferromagnetic interactions.
The first eight cobalt complexes of the pioneering ligand salicylhydroxamic acid have been established. Moreover, the cyclic scaffold of the new cobalt metallacrowns has been established as a versatile interface to SMM features based on a virtually magnetically isolated Co(II) ion by the realization of three novel single-molecule magnets with energy barriers of 14, 35 and 79 K. Static and dynamic magnetic measurements have enabled revealing magneto-structural correlations and provided new insights into the interplay between different relaxation processes.