Atomic-scale mechanism of grain boundary motion in graphene

Grain boundaries (GBs) in graphene can migrate when irradiated by electron beams from a transmission electron microscope (TEM). Here, we present an ab initio study on the atomic scale-mechanism for motion of GB with misorientation angle of ∼30° in graphene. From total energy calculations and energy barrier calculations, we find that a Stone–Wales (SW)-type transformation can occur more easily near GBs than in pristine graphene due to a reduced energy barrier of 7.23 eV; thus, this transformation is responsible for the motion of GBs. More interestingly, we find that a mismatch in the crystalline orientation at GBs can drive the evaporation of a carbon dimer by greatly reducing the corresponding overall energy barrier to 11.38 eV. After evaporation of the carbon dimer, the GBs can be stabilized through a series of SW-type transformations that result in GB motion. The GB motion induced by evaporation of the dimer is in excellent agreement with recent TEM experiments. Our findings elucidate the mechanism for the dynamics of GBs during TEM experiments and enhance the controllability of GBs in graphene.