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A systematic approach to mass-production of graphene and other 2D materials is essential for current and future technological applications. By combining a sequential statistical design of experiments with in-situ process monitoring, we demonstrate a method to optimize graphene growth on copper foil in a roll-to-roll rf plasma chemical vapor deposition system. Data-driven predictive models show that gas pressure, nitrogen, oxygen, and plasma power are the main process parameters affecting the quality of graphene. Furthermore, results from in-situ optical emission spectroscopy reveal a positive correlation of CH radical to high quality of graphene, whereas O and H atoms, Ar+ ion, and C2 and CN radicals negatively correlate to quality. This work demonstrates the deposition of graphene on copper foil at 1 m/min, a scale suitable for large-scale production. The techniques described here can be extended to other 2D materials and roll-to-roll manufacturing processes

Process optimization of graphene growth in a roll-to-roll plasma CVD system