Evangeli Charalambos, Tewari Sumit, Kruip Jonathan Marcell, Bian Xinya, Swett Jacob L, Cully John, Thomas James, Briggs G Andrew D, Mol Jan A
Department of Materials, University of Oxford, Oxford OX1 3PH, United Kingdom.
School of Physics and Astronomy, Queen Mary University of London, London E1 4NS, United Kingdom.
Proc Natl Acad Sci U S A. 2022 Jul 5;119(27):e2119015119. doi: 10.1073/pnas.2119015119. Epub 2022 Jun 27.
Controlled electrobreakdown of graphene is important for the fabrication of stable nanometer-size tunnel gaps, large-scale graphene quantum dots, and nanoscale resistive switches, etc. However, owing to the complex thermal, electronic, and electrochemical processes at the nanoscale that dictate the rupture of graphene, it is difficult to generate conclusions from individual devices. We describe here a way to explore the statistical signature of the graphene electrobreakdown process. Such analysis tells us that feedback-controlled electrobreakdown of graphene in the air first shows signs of joule heating-induced cleaning followed by rupturing of the graphene lattice that is manifested by the lowering of its conductance. We show that when the conductance of the graphene becomes smaller than around 0.1 , the effective graphene notch width starts to decrease exponentially slower with time. Further, we show how this signature gets modified as we change the environment and or the substrate. Using statistical analysis, we show that the electrobreakdown under a high vacuum could lead to substrate modification and resistive-switching behavior, without the application of any electroforming voltage. This is attributed to the formation of a semiconducting filament that makes a Schottky barrier with the graphene. We also provide here the statistically extracted Schottky barrier threshold voltages for various substrate studies. Such analysis not only gives a better understanding of the electrobreakdown of graphene but also can serve as a tool in the future for single-molecule diagnostics.
石墨烯的可控电击穿对于制造稳定的纳米尺寸隧道间隙、大规模石墨烯量子点和纳米级电阻开关等至关重要。然而,由于在纳米尺度上决定石墨烯破裂的复杂热、电子和电化学过程,很难从单个器件得出结论。我们在此描述一种探索石墨烯电击穿过程统计特征的方法。这种分析告诉我们,空气中石墨烯的反馈控制电击穿首先表现出焦耳热诱导清洁的迹象,随后是石墨烯晶格的破裂,这表现为其电导降低。我们表明,当石墨烯的电导小于约0.1时,有效石墨烯缺口宽度随时间开始以指数形式减慢减小。此外,我们展示了随着环境和/或衬底的变化,这种特征是如何改变的。通过统计分析,我们表明在高真空下的电击穿会导致衬底改性和电阻开关行为,而无需施加任何电形成电压。这归因于形成了与石墨烯形成肖特基势垒的半导体细丝。我们还在此提供了各种衬底研究中通过统计提取的肖特基势垒阈值电压。这种分析不仅能更好地理解石墨烯的电击穿,而且在未来还可作为单分子诊断的工具。