Reconstruction of Zigzag Graphene Edges: Energetics, Kinetics, and Residual Defects

Ab initio calculations are performed to study consecutive reconstruction of a zigzag graphene edge. According to the obtained energy profile along the reaction pathway, the first reconstruction step, formation of the first pentagon-heptagon pair, is the slowest one, while the growth of an already nucleated reconstructed edge domain should occur steadily at a much higher rate. Domains merge into one only in 1/4 of cases when they get in contact, while in the rest of the cases, residual defects are left. Structure, energy, and magnetic properties of these defects are studied. It is found that spontaneous formation of pairs of residual defects (i.e., spontaneous domain nucleation) in the fully reconstructed edge is unlikely at temperatures below 1000 K. Using a kinetic model, we show that the average domain length is several micrometers at room temperature and it decreases exponentially upon increasing the temperature at which the reconstruction takes place.