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Published June 20, 2017 | Supplemental Material + Accepted Version
Journal Article Open

Regulating Top-Surface Multilayer/Single-Crystal Graphene Growth by "Gettering" Carbon Diffusion at Backside of the Copper Foil

Abstract

A unique strategy is reported to constrain the nucleation centers for multilayer graphene (MLG) and, later, single-crystal graphene domains by gettering carbon source on backside of the flat Cu foil, during chemical vapor deposition. Hitherto, for a flat Cu foil, the top-surface-based growth mechanism is emphasized, while overlooking the graphene on the backside. However, the systematic experimental findings indicate a strong correlation between the backside graphene and the nucleation centers on the top-surface, governed by the carbon diffusion through the bulk Cu. This understanding steers to devise a strategy to mitigate the carbon diffusion to the top-surface by using a carbon "getter" substrate, such as nickel, on the backside of the Cu foil. Depth profiling of the nickel substrate, along with the density functional theory calculations, verifies the gettering role of the nickel support. The implementation of the backside carbon gettering approach on single-crystal graphene growth results in lowering the nucleation density by two orders of magnitude. This enables the single-crystal domains to grow by 6 mm laterally on the untreated Cu foil. Finally, the growth of large-area polycrystalline single layer graphene, free of unwanted MLG domains, with significantly improved field-effect mobility of ≈6800 cm^2 V^(−1) s^(−1) is demonstrated.

Additional Information

© 2017 Wiley-VCH Verlag GmbH & Co. Version of Record online: 11 Apr 2017. Manuscript Revised: 13 Feb 2017. Manuscript Received: 9 Jan 2017. This project was supported by the Research Grant Council of Hong Kong SAR (Project number 16204815). The authors appreciate the support from the Center for 1D/2D Quantum Materials and the Innovation and Technology Commission (ITC-CNERC14SC01). I.H.A. appreciates financial support from the Higher Education Commission (HEC) of Pakistan. Technical assistance from the Materials Characterization and Preparation Facilities is greatly appreciated. Y.L. thanks the support from the Resnick Prize Postdoctoral Fellowship at the Caltech. W.A.G. III thanks the NSF (DMREF-1436985) and the DOE (DE-SC0014607) for support. This work used computational resources provided by the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract DE-AC02-05CH11231, the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by the NSF Grant ACI-1053575, and of the National Renewable Energy Laboratory supported by the DoE office of Energy Efficiency and Renewable Energy.

Attached Files

Accepted Version - RegulatingGraphene_Growth_Gettering-final.pdf

Supplemental Material - adfm201700121-sup-0001-S1.pdf

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August 19, 2023
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