Reproducible graphene synthesis by oxygen-free chemical vapour deposition

Chemical vapour deposition (CVD) synthesis of graphene on copper has been broadly adopted since the first demonstration of this process1. However, widespread use of CVD-grown graphene for basic science and applications has been hindered by challenges with reproducibility2 and quality3. Here we identify trace oxygen as a key factor determining the growth trajectory and quality for graphene grown by low-pressure CVD. Oxygen-free chemical vapour deposition (OF-CVD) synthesis is fast and highly reproducible, with kinetics that can be described by a compact model, whereas adding trace oxygen leads to suppressed nucleation and slower/incomplete growth. Oxygen affects graphene quality as assessed by surface contamination, emergence of the Raman D peak and decrease in electrical conductivity. Epitaxial graphene grown in oxygen-free conditions is contamination-free and shows no detectable D peak. After dry transfer and boron nitride encapsulation, it shows room-temperature electrical-transport behaviour close to that of exfoliated graphene. A graphite-gated device shows well-developed integer and fractional quantum Hall effects. By highlighting the importance of eliminating trace oxygen, this work provides guidance for future CVD system design and operation. The increased reproducibility and quality afforded by OF-CVD synthesis will broadly influence basic research and applications of graphene.