Tension-controlled single-crystallization of copper foils for roll-to-roll synthesis of high-quality graphene films

It has been known that the crystalline orientation of Cu substrates plays a crucial role in chemical vapor deposition (CVD) synthesis of high-quality graphene. In particular, Cu (1 1 1) surface showing the minimum lattice mismatch with graphene is expected to provide an ideal catalytic reactivity that can minimize the formation of defects, which also induces larger single-crystalline domain sizes of graphene. Usually, the Cu (1 1 1) substrates can be epitaxially grown on single-crystalline inorganic substrates or can be recrystallized by annealing for more than 12 h, which limits the cost and time-effective synthesis of graphene. Here, we demonstrate a new method to optimize the crystalline orientations of vertically suspended Cu foils by tension control during graphene growth, resulting in large-area recrystallization into Cu (1 1 1) surface as the applied tension activates the grain boundary energy of Cu and promotes its abnormal grain growth to single crystals. In addition, we found a clue that the formation of graphene cooperatively assists the recrystallization into Cu (1 1 1) by minimizing the surface energy of Cu. The domain sizes and charge carrier mobility of graphene grown on the single-crystalline Cu (1 1 1) are 5 times and ~50% increased, respectively, in comparison with those of graphene from Cu (1 0 0), indicating that the less lattice mismatch and the lower interaction energy between Cu (1 1 1) and graphene allows the growth of larger single-crystalline graphene with higher charge carrier mobility. Thus, we believe that our finding provides a crucial idea to design a roll-to-roll (R2R) graphene synthesis system where the tension control is inevitably involved, which would be of great importance for the continuous production of high-quality graphene in the future.