Ab initio quantum transport in polycrystalline graphene

Synthesis techniques such as chemical vapor deposition yield graphene in polycrystalline flakes where single-crystal domains are separated by grain boundaries (GBs) of irregular shape. These structural defects are mostly made up of pentagon-heptagon pairs and represent an important source of scattering, thus strongly affecting electronic mobilities in polycrystalline graphene (PG). In the present article, first-principles simulations are performed to explore charge transport through a GB in PG using the Landauer-Buttiker formalism implemented within the Green's function approach. In ideal GB configurations, electronic transport is found to depend on their topology as already suggested in the literature. However, more realistic GBs constructed out of various carbon rings and with more complex periodicities are also considered, possibly inducing leakage currents. Finally, additional realistic disorder such as vacancies, a larger inter-connectivity region and out-of plane buckling is investigated. For specific energies, charge redistribution effects related to the detailed GB topology are found to substantially alter the transmissions. Altogether, the transport gap is predicted to be inversely proportional to the smallest significant periodic pattern and nearly independent of the interface configuration.