Anomalous Strength Characteristics of Tilt Grain Boundaries in Graphene

Using molecular dynamics simulations and first principles calculations, we have studied the structure and mechanical strength of tilt grain boundaries in graphene sheets that arise during CVD growth of graphene on metal substrates. Surprisingly, we find that for tilt boundaries in the vicinity of both the zig-zag and arm-chair orientations, large angle boundaries with a higher density of 5-7 defect pairs are stronger than the low-angle boundaries which are comprised of fewer defects per unit length. Interestingly, the trends in our results cannot be explained by a continuum Griffith-type fracture mechanics criterion, which predicts the opposite trend due to that fact that it does not account for the critical bonds that are responsible for the failure mechanism. We have identified the highly-strained bonds in the 7-member rings that lead to the failure of the sheets, and we have found that large angle boundaries are able to better accommodate the strained 7-rings. Our results provide guidelines for designing growth methods to obtain grain boundary structures that can have strengths close to that of pristine graphene.