Department of Mechanical Engineering, Columbia University, New York, NY, USA.
Infinite Potential Laboratories, Waterloo, Ontario, Canada.
Nature. 2024 Jun;630(8017):636-642. doi: 10.1038/s41586-024-07454-5. Epub 2024 May 29.
Chemical vapour deposition (CVD) synthesis of graphene on copper has been broadly adopted since the first demonstration of this process. However, widespread use of CVD-grown graphene for basic science and applications has been hindered by challenges with reproducibility and quality. 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.
化学气相沉积(CVD)在铜上合成石墨烯自该工艺首次展示以来已被广泛采用。然而,由于重复性和质量的挑战,CVD 生长的石墨烯在基础科学和应用中的广泛应用受到了阻碍。在这里,我们确定痕量氧是决定通过低压 CVD 生长的石墨烯的生长轨迹和质量的关键因素。无氧气化学气相沉积(OF-CVD)合成速度快且重复性高,动力学可以用一个紧凑的模型来描述,而添加痕量氧会抑制成核并减缓/不完全生长。氧通过表面污染、拉曼 D 峰的出现和电导率的降低来影响石墨烯的质量。在无氧条件下生长的外延石墨烯无污染,没有可检测到的 D 峰。经过干法转移和氮化硼封装后,它表现出接近剥离石墨烯的室温输运行为。石墨栅极器件表现出良好的整数和分数量子霍尔效应。通过强调消除痕量氧的重要性,这项工作为未来的 CVD 系统设计和操作提供了指导。OF-CVD 合成提供的更高的重复性和质量将广泛影响石墨烯的基础研究和应用。