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High versus low : The high‐yield generation of a synthetic high‐spin oxoiron(IV) complex, [FeIV(O)(TMG3tren)]2+ (see picture, TMG3tren = 1,1,1‐tris{2‐[N2‐(1,1,3,3‐tetramethylguanidino)]ethyl}amine), has been achieved by using the very bulky tetradentate TMG3tren ligand, in order to both sterically protect the oxoiron(IV) moiety and enforce a trigonal bipyramidal geometry at the iron center, for which an S=2 ground state is favored.

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