Robust Room Temperature Ferromagnetism In Cobalt Doped Graphene by Precision Control of Metal Ion Hybridization

Abstract Graphene‐based magnetic materials exhibit novel properties and promising applications in the development of next‐generation spintronic devices. Modern synthesis techniques have paved the way to design precisely the local environments of metal atoms anchored onto a nitrogen‐doped graphene matrix. Herein, it is demonstrated that grafting cobalt (Co) into the graphene lattice induces robust and stable room‐temperature ferromagnetism. These comprehensive experiments and first‐principles calculations unambiguously identify that the mechanism for this unusual ferromagnetism is π‐d orbital hybridization between Co dxz and graphene pz orbitals. Here, it is found that the magnetic interactions of Co–carbon ions are mediated by the spin‐polarized graphene pz orbitals, and room temperature ferromagnetism can be stabilized by electron doping. It is also found that the electronic structure n…