期刊
CARBON
卷 107, 期 -, 页码 857-864出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.carbon.2016.06.091
关键词
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资金
- Ministry of Science and Technology (MoST) of Taiwan [MoST 104-2112-M-032-002-MY3, NSC 102-2632-M-032-001-MY3]
- NCTS of Taiwan
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- Natural Sciences and Engineering Research Council of Canada
- National Research Council Canada
- Canadian Institutes of Health Research
- Province of Saskatchewan
- Western Economic Diversification Canada
- University of Saskatchewan
We have demonstrated a nonlinear behavior for the bandgap opening of doped graphene by controlling the concentration of B and N co-dopants. X-ray absorption and emission spectra reveal that the bandgap increases from 0 to 0.6 eV as the concentration of BN dopants is increased from 0 to 6%, while the bandgap closes when the doping concentration becomes 56%. This nonlinear behavior of bandgap opening of the BN-doped graphene depending on the BN concentrations is consistent with the valenceband photoemission spectroscopic measurements. The spatially resolved B, N and C K-edge scanning transmission x-ray microscopy and their x-ray absorption near- edge structure spectra all support the scenario of the development of h-BN-like domains at high concentrations of BN. Ab initio calculation, by taking into account of the strong correlation between the bandgap and the geometry/concentration of the dopant, has been performed with various BN-dopant nano-domains embedded in the graphene monolayer to verify the unique bandgap behavior. Based on the experimental measurements and ab initio calculation, we propose the progressive formation of a phase-separated zigzag-edged BN domain from BN quantum dots with increasing BN-dopant concentration to explain the extraordinary nonlinear behavior of bandgap opening of BN-doped graphene sheets. This study reveals a new way to engineer the bandgap of low-dimensional systems. (C) 2016 Elsevier Ltd. All rights reserved.
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