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Magnetic order emerging in otherwise non-magnetic materials as carbon is aparadigmatic example of a novel type of s-p electron magnetism predicted to beof exceptional high-temperature stability. It has been demonstrated that atomicscale structural defects of graphene can host unpaired spins. However, it isstill unclear under which conditions long-range magnetic order can emerge fromsuch defect-bound magnetic moments. Here we propose that in contrast to randomdefect distributions, atomic scale engineering of graphene edges with specificcrystallographic orientation, comprising edge atoms only from one sub-latticeof the bipartite graphene lattice, can give rise to a robust magnetic order. Weemploy a nanofabrication technique based on Scanning Tunneling Microscopy todefine graphene nanoribbons with nanometer precision and well-definedcrystallographic edge orientations. While armchair ribbons display quantumconfinement gap, zigzag ribbons narrower than 7 nm reveal a bandgap of about0.2 - 0.3 eV, which can be identified as a signature of interaction inducedspin ordering along their edges. Moreover, a semiconductor to metal transitionis revealed upon increasing the ribbon width, indicating the switching of themagnetic coupling between opposite ribbon edges from antiferromagnetic toferromagnetic configuration. We found that the magnetic order on graphene edgesof controlled zigzag orientation can be stable even at room temperature,raising hope for graphene-based spintronic devices operating under ambientconditions.

Room temperature magnetic order on zigzag edges of narrow graphene nanoribbons