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Single-crystal, large-area, fold-free monolayer graphene

Meihui Wang, Ming Huang, Da Luo (), Yunqing Li, Myeonggi Choe, Won Kyung Seong, Minhyeok Kim, Sunghwan Jin, Mengran Wang, Shahana Chatterjee, Youngwoo Kwon, Zonghoon Lee and Rodney S. Ruoff ()
Additional contact information
Meihui Wang: Institute for Basic Science (IBS)
Ming Huang: Institute for Basic Science (IBS)
Da Luo: Institute for Basic Science (IBS)
Yunqing Li: Institute for Basic Science (IBS)
Myeonggi Choe: Institute for Basic Science (IBS)
Won Kyung Seong: Institute for Basic Science (IBS)
Minhyeok Kim: Institute for Basic Science (IBS)
Sunghwan Jin: Institute for Basic Science (IBS)
Mengran Wang: Institute for Basic Science (IBS)
Shahana Chatterjee: Institute for Basic Science (IBS)
Youngwoo Kwon: Institute for Basic Science (IBS)
Zonghoon Lee: Institute for Basic Science (IBS)
Rodney S. Ruoff: Institute for Basic Science (IBS)

Nature, 2021, vol. 596, issue 7873, 519-524

Abstract: Abstract Chemical vapour deposition of carbon-containing precursors on metal substrates is currently the most promising route for the scalable synthesis of large-area, high-quality graphene films1. However, there are usually some imperfections present in the resulting films: grain boundaries, regions with additional layers (adlayers), and wrinkles or folds, all of which can degrade the performance of graphene in various applications2–7. There have been numerous studies on ways to eliminate grain boundaries8,9 and adlayers10–12, but graphene folds have been less investigated. Here we explore the wrinkling/folding process for graphene films grown from an ethylene precursor on single-crystal Cu–Ni(111) foils. We identify a critical growth temperature (1,030 kelvin) above which folds will naturally form during the subsequent cooling process. Specifically, the compressive stress that builds up owing to thermal contraction during cooling is released by the abrupt onset of step bunching in the foil at about 1,030 kelvin, triggering the formation of graphene folds perpendicular to the step edge direction. By restricting the initial growth temperature to between 1,000 kelvin and 1,030 kelvin, we can produce large areas of single-crystal monolayer graphene films that are high-quality and fold-free. The resulting films show highly uniform transport properties: field-effect transistors prepared from these films exhibit average room-temperature carrier mobilities of around (7.0 ± 1.0) × 103 centimetres squared per volt per second for both holes and electrons. The process is also scalable, permitting simultaneous growth of graphene of the same quality on multiple foils stacked in parallel. After electrochemical transfer of the graphene films from the foils, the foils themselves can be reused essentially indefinitely for further graphene growth.

Date: 2021
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DOI: 10.1038/s41586-021-03753-3

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