Reproducible graphene synthesis by oxygen-free chemical vapour deposition

Jacob Amontree, Xingzhou Yan, Christopher S. DiMarco, Pierre L. Levesque, Tehseen Adel, Jordan Pack, Madisen Holbrook, Christian Cupo, Zhiying Wang, Dihao Sun, Adam J. Biacchi, Charlezetta E. Wilson-Stokes, Kenji Watanabe, Takashi Taniguchi, Cory R. Dean, Angela R. Hight Walker, Katayun Barmak (), Richard Martel () and James Hone ()
Additional contact information
Jacob Amontree: Columbia University
Xingzhou Yan: Columbia University
Christopher S. DiMarco: Columbia University
Pierre L. Levesque: Infinite Potential Laboratories
Tehseen Adel: National Institute of Standards and Technology (NIST)
Jordan Pack: Columbia University
Madisen Holbrook: Columbia University
Christian Cupo: Columbia University
Zhiying Wang: Columbia University
Dihao Sun: Columbia University
Adam J. Biacchi: National Institute of Standards and Technology (NIST)
Charlezetta E. Wilson-Stokes: National Institute of Standards and Technology (NIST)
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Cory R. Dean: Columbia University
Angela R. Hight Walker: National Institute of Standards and Technology (NIST)
Katayun Barmak: Columbia University
Richard Martel: Université de Montréal
James Hone: Columbia University

Nature, 2024, vol. 630, issue 8017, 636-642

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41586-024-07454-5

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