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Cu has shown an advantage in growing monolayer graphene due to the very low C solubility and surface-mediated self-limiting growth, which hinders the growth of multilayer graphene. This work reports an unconventional penetration etching/growth of graphene adlayers tuned by oxygen beyond the self-limiting growth, supported by the C isotope labeling results. The effect of oxygen is nonmonotonic, i.e., with the increase of oxygen, graphene adlayers are etched without damaging the top layer, then shift to growth, and finally, all layers are etched. In addition, the reaction did not seem to reach equilibrium in the time range of the experiment but continued as if oxygen was increasing with respect to time. An oxygen-assisted exchange penetration model is proposed to interpret the growth mechanism. Oxygen etches the top shield layer, which is simultaneously healed by consuming the C species around adlayers and results in adlayer decomposition due to the break of equilibrium. Additionally, oxygen assists penetration of C from the gaseous agents into the shield layer for adlayer growth. The domination of one over the other depends on the concentration of oxygen, resulting in overall etching or growth. Finally, the synthesis of large-area monolayer and bilayer graphene films with good uniformity is demonstrated.

The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adem.202201311.

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