A unique strategy is reported to constrain the nucleation centers for multilayer graphene (MLG) and, later, single‐crystal graphene domains by gettering carbon source on backside of the flat Cu foil, during chemical vapor deposition. Hitherto, for a flat Cu foil, the top‐surface‐based growth mechanism is emphasized, while overlooking the graphene on the backside. However, the systematic experimental findings indicate a strong correlation between the backside graphene and the nucleation centers on the top‐surface, governed by the carbon diffusion through the bulk Cu. This understanding steers to devise a strategy to mitigate the carbon diffusion to the top‐surface by using a carbon “getter” substrate, such as nickel, on the backside of the Cu foil. Depth profiling of the nickel substrate, along with the density functional theory calculations, verifies the gettering role of the nickel support. The implementation of the backside carbon gettering approach on single‐crystal graphene growth results in lowering the nucleation density by two orders of magnitude. This enables the single‐crystal domains to grow by 6 mm laterally on the untreated Cu foil. Finally, the growth of large‐area polycrystalline single layer graphene, free of unwanted MLG domains, with significantly improved field‐effect mobility of ≈6800 cm2 V−1 s−1 is demonstrated.
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