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Exposing graphene to a hydrogen post-etching process yields dendritic graphene shapes. Here, we demonstrate that similar dendritic structures can be achieved at long growth times without adding hydrogen externally. These shapes are not a result of a surface diffusion controlled growth but of the competing backward reaction (etching), which dominates the growth dynamics at long times due to an in situ rise in the hydrogen partial pressure. We have performed a systematic study on the growth of graphene as a function of time to identify the onset and gradual evolution of graphene shapes caused by etching and then demonstrated that the etching can be stopped by reducing the flow of hydrogen from the feed. In addition, we have found that the etching rate due to the in situ rise in hydrogen is strongly dependent on the confinement (geometrical confinement) of copper foil. Highly etched graphene with dendritic shapes was observed in unconfined copper foil regions while no etching was found in graphene grown in a confined reaction region. This highlights the effect of the dynamic reactant distribution in activating the in situ etching process during growth, which needs to be counteracted or controlled for large scale growth.

Impact of the in situ rise in hydrogen partial pressure on graphene shape evolution during CVD growth of graphene