Redox-modulated switching of ferro to antiferromagnetic coupling in endohedral fullerenes: A broken-symmetry approach

•Molecular magnets based on charged endohedral fullerenes.•Change of sign and magnitude of J during the redox process.•Potency of N@C60 in designing redox-governed magnetic switches.

The redox-governed switching potency from ferro to antiferromagnetic coupling and vice versa of three already synthesized endohedral fullerenes N@C60, N@C70 and P@C60 has been studied using the broken symmetry method. The calculated exchange coupling constants for cation and anion forms of N@C60 indicate ferro and antiferromagnetic interactions respectively. In this work, several pure and hybrid functionals were examined on N@C60 to study the amount of Hartree-Fock exact exchange effect in magnetic exchange coupling constant values. Furthermore, the spin density distributions and molecular orbitals shapes have been analyzed to explain the nature of exchange-coupling interactions and their pathways respectively.

Graphical abstractDownload high-res image (96KB)Download full-size image