Molecular dynamics (MD) simulations are used to gain insights into the process conditions that cause separation of graphene layers from a highly ordered pyrolytic graphite (HOPG) source in a polydimethylsiloxane (PDMS) stamp-assisted mechanical exfoliation process. Specifically, the effects of selected exfoliation process parameters and pre-existing defects, such as layer discontinuities in the graphite source, on the exfoliation process are investigated. The results show that exfoliation of individual and few layer graphene requires delicate control of the normal force applied to the HOPG by the PDMS stamp. The study also shows that defects (e.g., discontinuities) in the HOPG have a significant impact on the thickness of separated layers and the layer separation force. The insights derived from this study are expected to be very useful in the development of a low-cost, scalable, large area graphene production process.

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