Design of Molecular Scaffolds Based on Unusual Geometries for Magnetic Modulation of Spin-Diverse Complexes with Selective Redox Response

A weakly coupled heterometallic [CuFe] complex has been prepared in which the metal centers are coordinated to a new electroactive ligand. The spin-diverse system delivers distinct ground states upon application of selective redox potentials. Ligand oxidation fosters radical generation, and the initial ground state associated with a weakly coupled [CuFe] core switches to a ground state associated with the [Fe−radical] coupling; the Cu(II) ion remains uncoupled. A third state is obtained upon reduction of the cupric center and in absence of the radical. The possibilities and limitations of these systems are discussed.