Large‐Scale Synthesis of Bi‐layer Graphene in Strongly Coupled Stacking Order

Abstract Large‐scale synthesis of single‐layer graphene (SLG) by chemical vapor deposition (CVD) has received a lot of attention recently. However, CVD synthesis of AB stacked bi‐layer graphene (BLG) is still challenging. Here, we report synthesis of BLG homogeneously at large scale by thermal CVD. The 2D Raman band of CVD BLG splits into four components, suggesting splitting of electronic bands due to strong interlayer coupling. The splitting of electronic bands in CVD BLG is further evidenced by the study of near infrared absorption and carrier dynamics are probed by transient absorption spectroscopy. UV photoelectron spectroscopy invesigation also indiates CVD BLG possesses different electronic structures to those of CVD SLG. The growth mechanism of BLG is found to be related to catalytic activity of the copper (Cu) surface, which is determined by the purity of Cu foils employed in the CVD process. Our work shows that strongly coupled or even AB stacked BLG can be grown on Cu foils at large scale, which is of particular importance for device applications based on their split electronic bands.