Abstract

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.

Highlights

  • Two-dimensional (2D) materials, such as graphene, hexagonal boron nitride (h-BN) and transition metal dichalcogenides (TMDs) have attracted immense attention in the past decade.1,2 2D materials possess a range of favorable properties, from the zero band-gap and high electrical, and thermal conductivity of graphene[3,4] to the wide band gap and good dielectric properties of h-BN.[5,6] Several studies have considered mass-production of graphene using a variety of techniques.[7]

  • Utilizing the advantages of the roll-to-roll process, multiple experiments were conducted in one set with negligible influence of experimental sequence on graphene deposition

  • After starting with initial sets of random measurements, called Sets 1-3 in Fig. 4, the methodology selects the conditions of the seven process parameters to maximize the quality and information in the Pareto efficient frontier (PEF)

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Summary

Introduction

Two-dimensional (2D) materials, such as graphene, hexagonal boron nitride (h-BN) and transition metal dichalcogenides (TMDs) have attracted immense attention in the past decade.1,2 2D materials possess a range of favorable properties, from the zero band-gap and high electrical, and thermal conductivity of graphene[3,4] to the wide band gap and good dielectric properties of h-BN.[5,6] Several studies have considered mass-production of graphene using a variety of techniques.[7]. Exfoliation produces low yields,[9] requires high energy input[9] and produces graphene sheets with structural defects. Another method for large-scale production of graphene is chemical vapor deposition (CVD) which has been proven to produce higher quality, large-area, single and few-layer graphene films.[11].

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