Controlling edge morphology in graphene layers using electron irradiation: From sharp atomic edges to coalesced layers forming loops

Recent experimental reports indicate that Joule heating can atomically sharpen the edges of chemical vapor deposition grown graphitic nanoribbons. The absence or presence of loops between adjacent layers in the annealed materials is the topic of a growing debate that this Letter aims to put to rest. We offer a rationale explaining why loops do form if Joule heating is used alone, and why adjacent nanoribbon layers do not coalesce when Joule heating is applied after high-energy electrons first irradiate the sample. Our work, based on large-scale quantum molecular dynamics and electronic-transport calculations, shows that vacancies on adjacent graphene sheets, created by electron irradiation, inhibit the formation of edge loops.