Imprinting Tunable π-Magnetism in Graphene Nanoribbons via Edge Extensions

Magnetic carbon nanostructures are currently under scrutiny for a wide spectrum of applications. Here, we theoretically investigate armchair graphene nanoribbons patterned with asymmetric edge extensions consisting of laterally fused naphtho groups, as recently fabricated via on-surface synthesis. We show that an individual edge extension acts as a spin-$$ center and develops a sizable spin-polarization of the conductance around the band edges. The Heisenberg exchange coupling between a pair of edge extensions is dictated by the position of the second naphtho group in the carbon backbone, thus enabling ferromagnetic, antiferromagnetic, or nonmagnetic states. The periodic arrangement of edge extensions yields full spin-polarization at the band extrema, and the accompanying ferromagnetic ground state can be driven into nonmagnetic or antiferromagnetic phases through external stimuli. Overall, our work reveals a precise tunability of the π-magnetism in graphene nanoribbons induced by naphtho groups, thereby establishing these one-dimensional architectures as suitable platforms for logic spintronics.