Defect engineering of graphene using electron-beam chemistry with radiolyzed water

Abstract

Defect engineering of graphene is attractive for a wide range of applications. Here, we present a mask-less, resist-free, and fully reversible process to engineer defects in graphene using electron-beam (e-beam) chemistry with radiolyzed water. This process was performed inside a variable pressure scanning electron microscope by generating radiolysis products using reactions between the e-beam and water vapor, which in turn reacted with the graphene at the location of the probe. These reactions enabled controlled chemistry on the graphene surface at a resolution of ∼60 nm and hence created defects in precise locations defined by the e-beam. Detailed characterization and theoretical analyses suggested the presence of sp3-type defects, the density of which was tuned by varying the e-beam dose. In addition, these sp3-type defects were cycled in and out of graphene by alternating e-beam chemistry and thermal annealing. This reversibility promises future applications of e-beam chemistry in reconfigurable plasmonics and electronics.