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Title: Oxygen-activated growth and bandgap tunability of large single-crystal bilayer graphene

Abstract

Bernal (AB)-stacked bilayer graphene (BLG) is a semiconductor whose bandgap can be tuned by a transverse electric field, making it a unique material for a number of electronic and photonic devices. A scalable approach to synthesize high-quality BLG is therefore critical, which requires minimal crystalline defects in both graphene layers and maximal area of Bernal stacking, which is necessary for bandgap tunability. Here we demonstrate that in an oxygen-activated chemical vapour deposition (CVD) process, half-millimetre size, Bernal-stacked BLG single crystals can be synthesized on Cu. Besides the traditional 'surface-limited' growth mechanism for SLG (1st layer), we discovered new microscopic steps governing the growth of the 2nd graphene layer below the 1st layer as the diffusion of carbon atoms through the Cu bulk after complete dehydrogenation of hydrocarbon molecules on the Cu surface, which does not occur in the absence of oxygen. Moreover, we found that the efficient diffusion of the carbon atoms present at the interface between Cu and the 1st graphene layer further facilitates growth of large domains of the 2nd layer. The CVD BLG has superior electrical quality, with a device on/off ratio greater than 104, and a tunable bandgap up to -100 meV at a displacement fieldmore » of 0.9 V nm-1.« less

Authors:
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Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1253273
Report Number(s):
NREL/JA-5900-65891
Journal ID: ISSN 1748-3387
DOE Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article
Journal Name:
Nature Nanotechnology
Additional Journal Information:
Journal Volume: 11; Journal Issue: 5; Related Information: Nature Nanotechnology; Journal ID: ISSN 1748-3387
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; electronic devices; electronic properties and devices; synthesis of graphene

Citation Formats

Hao, Yufeng, Wang, Lei, Liu, Yuanyue, Chen, Hua, Wang, Xiaohan, Tan, Cheng, Nie, Shu, Suk, Ji Won, Jiang, Tengfei, Liang, Tengfei, Xiao, Junfeng, Ye, Wenjing, Dean, Cory R., Yakobson, Boris I., McCarty, Kevin F., Kim, Philip, Hone, James, Colombo, Luigi, and Ruoff, Rodney S. Oxygen-activated growth and bandgap tunability of large single-crystal bilayer graphene. United States: N. p., 2016. Web. doi:10.1038/nnano.2015.322.
Hao, Yufeng, Wang, Lei, Liu, Yuanyue, Chen, Hua, Wang, Xiaohan, Tan, Cheng, Nie, Shu, Suk, Ji Won, Jiang, Tengfei, Liang, Tengfei, Xiao, Junfeng, Ye, Wenjing, Dean, Cory R., Yakobson, Boris I., McCarty, Kevin F., Kim, Philip, Hone, James, Colombo, Luigi, & Ruoff, Rodney S. Oxygen-activated growth and bandgap tunability of large single-crystal bilayer graphene. United States. doi:10.1038/nnano.2015.322.
Hao, Yufeng, Wang, Lei, Liu, Yuanyue, Chen, Hua, Wang, Xiaohan, Tan, Cheng, Nie, Shu, Suk, Ji Won, Jiang, Tengfei, Liang, Tengfei, Xiao, Junfeng, Ye, Wenjing, Dean, Cory R., Yakobson, Boris I., McCarty, Kevin F., Kim, Philip, Hone, James, Colombo, Luigi, and Ruoff, Rodney S. Mon . "Oxygen-activated growth and bandgap tunability of large single-crystal bilayer graphene". United States. doi:10.1038/nnano.2015.322.
@article{osti_1253273,
title = {Oxygen-activated growth and bandgap tunability of large single-crystal bilayer graphene},
author = {Hao, Yufeng and Wang, Lei and Liu, Yuanyue and Chen, Hua and Wang, Xiaohan and Tan, Cheng and Nie, Shu and Suk, Ji Won and Jiang, Tengfei and Liang, Tengfei and Xiao, Junfeng and Ye, Wenjing and Dean, Cory R. and Yakobson, Boris I. and McCarty, Kevin F. and Kim, Philip and Hone, James and Colombo, Luigi and Ruoff, Rodney S.},
abstractNote = {Bernal (AB)-stacked bilayer graphene (BLG) is a semiconductor whose bandgap can be tuned by a transverse electric field, making it a unique material for a number of electronic and photonic devices. A scalable approach to synthesize high-quality BLG is therefore critical, which requires minimal crystalline defects in both graphene layers and maximal area of Bernal stacking, which is necessary for bandgap tunability. Here we demonstrate that in an oxygen-activated chemical vapour deposition (CVD) process, half-millimetre size, Bernal-stacked BLG single crystals can be synthesized on Cu. Besides the traditional 'surface-limited' growth mechanism for SLG (1st layer), we discovered new microscopic steps governing the growth of the 2nd graphene layer below the 1st layer as the diffusion of carbon atoms through the Cu bulk after complete dehydrogenation of hydrocarbon molecules on the Cu surface, which does not occur in the absence of oxygen. Moreover, we found that the efficient diffusion of the carbon atoms present at the interface between Cu and the 1st graphene layer further facilitates growth of large domains of the 2nd layer. The CVD BLG has superior electrical quality, with a device on/off ratio greater than 104, and a tunable bandgap up to -100 meV at a displacement field of 0.9 V nm-1.},
doi = {10.1038/nnano.2015.322},
journal = {Nature Nanotechnology},
issn = {1748-3387},
number = 5,
volume = 11,
place = {United States},
year = {2016},
month = {2}
}