Room temperature magnetic order on zigzag edges of narrow graphene nanoribbons

Abstract: Magnetic order emerging in otherwise non-magnetic materials as carbon is a paradigmatic example of a novel type of s-p electron magnetism predicted to be of exceptional high-temperature stability. It has been demonstrated that atomic scale structural defects of graphene can host unpaired spins. However, it is still unclear under which conditions long-range magnetic order can emerge from such defect-bound magnetic moments. Here we propose that in contrast to random defect distributions, atomic scale engineering of graphene edges with specific crystallographic orientation, comprising edge atoms only from one sub-lattice of the bipartite graphene lattice, can give rise to a robust magnetic order. We employ a nanofabrication technique based on Scanning Tunneling Microscopy to define graphene nanoribbons with nanometer precision and well-defined crystallographic edge orientations. While armchair ribbons display quantum confinement gap, zigzag ribbons narrower than 7 nm reveal a bandgap of about 0.2 - 0.3 eV, which can be identified as a signature of interaction induced spin ordering along their edges. Moreover, a semiconductor to metal transition is revealed upon increasing the ribbon width, indicating the switching of the magnetic coupling between opposite ribbon edges from antiferromagnetic to ferromagnetic configuration. We found that the magnetic order on graphene edges of controlled zigzag orientation can be stable even at room temperature, raising hope for graphene-based spintronic devices operating under ambient conditions.