Bound and free self-interstitial defects in graphite and bilayer graphene: A computational study

The role of self-interstitials in the response of layered carbon materials such as graphite, bilayer graphene and multiwalled carbon nanotubes to irradiation has long remained a puzzle. Using density-functional-theory methods with an exchange and correlation functional which takes into account the interlayer van der Waals interaction in these systems without any material-specific empirical parameters, we study the energetics and migration of single- and di-interstitials in graphite and bilayer graphene. We show that two classes of interstitials, “bound” and “free,” can coexist. The latter are mobile at room and lower temperatures, which explains the experimental data and reconciles them with the results of atomistic simulations. Our results shed light on the behavior of graphite and carbon nanotubes under irradiation and have implications for irradiation-mediated processing of bilayer graphene.