Crown graphene nanomeshes: Highly stable chelation-doped semiconducting materials

Graphene nanomeshes (GNMs) formed by the creation of pore superlattices in graphene are a possible route to graphene-based electronics due to their semiconducting properties, including the emergence of fractional electronvolt band gaps. The utility of GNMs would be markedly increased if a scheme to stably and controllably dope them was developed. In this work, a chemically motivated approach to GNM doping based on selective pore-perimeter passivation and subsequent ion chelation is proposed. It is shown by first-principles calculations that ion chelation leads to stable doping of the passivated GNMs - both n- and p-doping are achieved within a rigid-band picture. Such chelated or "crown" GNM structures are stable, high mobility semiconducting materials possessing intrinsic doping-concentration control; these can serve as building blocks for edge-free graphene nanoelectronics including GNM-based complementary metal oxide semiconductor (CMOS)-type logic switches. © 2013 American Chemical Society.