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Title: Crystalline Bilayer Graphene with Preferential Stacking from Ni–Cu Gradient Alloy

Abstract

We developed a high-yield synthesis of highly crystalline bilayer graphene (BLG) with two preferential stacking modes using a Ni–Cu gradient alloy growth substrate. Previously reported approaches for BLG growth include flat growth substrates of Cu or Ni–Cu uniform alloys and “copper pocket” structures. Use of flat substrates has the advantage of being scalable, but the growth mechanism is either “surface limited” (for Cu) or carbon precipitation (for uniform Ni–Cu), which results in multicrystalline BLG grains. For copper pockets, growth proceeds through a carbon back-diffusion mechanism, which leads to the formation of highly crystalline BLG, but scaling of the copper pocket structure is expected to be difficult. Here we demonstrate a Ni–Cu gradient alloy that combines the advantages of these earlier methods: the substrate is flat, so easy to scale, while growth proceeds by a carbon back-diffusion mechanism leading to high-yield growth of BLG with high crystallinity. Here, the BLG layer stacking was almost exclusively Bernal or twisted with an angle of 30°, consistent with first-principles calculations we conducted. Furthermore, we demonstrated scalable production of transistor arrays based crystalline Bernal-stacked BLG with a band gap that was tunable at room temperature.

Authors:
 [1];  [2];  [1];  [3];  [4];  [1];  [5];  [1];  [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [6]; ORCiD logo [1]
  1. Univ. of Pennsylvania, Philadelphia, PA (United States)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States); Hong Kong Univ. of Science and Technology, Kowloon (Hong Kong)
  3. Univ. of Pennsylvania, Philadelphia, PA (United States); Sungkyunkwan Univ., Suwon (Korea)
  4. Hong Kong Univ. of Science and Technology, Kowloon (Hong Kong)
  5. Univ. of Pennsylvania, Philadelphia, PA (United States); Univ. San Francisco de Quito, Quito (Ecuador)
  6. South China Univ. of Technology, Guangzhou (People’s Republic of China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE
OSTI Identifier:
1488924
Grant/Contract Number:  
FG02-07ER46431
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 3; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
Bernal and 30° stacking order; bilayer graphene; high-yield synthesis; Ni−Cu gradient alloy; single-crystal

Citation Formats

Gao, Zhaoli, Zhang, Qicheng, Naylor, Carl H., Kim, Youngkuk, Abidi, Irfan Haider, Ping, Jinglei, Ducos, Pedro, Zauberman, Jonathan, Zhao, Meng -Qiang, Rappe, Andrew M., Luo, Zhengtang, Ren, Li, and Johnson, Alan T. Charlie. Crystalline Bilayer Graphene with Preferential Stacking from Ni–Cu Gradient Alloy. United States: N. p., 2018. Web. doi:10.1021/acsnano.7b06992.
Gao, Zhaoli, Zhang, Qicheng, Naylor, Carl H., Kim, Youngkuk, Abidi, Irfan Haider, Ping, Jinglei, Ducos, Pedro, Zauberman, Jonathan, Zhao, Meng -Qiang, Rappe, Andrew M., Luo, Zhengtang, Ren, Li, & Johnson, Alan T. Charlie. Crystalline Bilayer Graphene with Preferential Stacking from Ni–Cu Gradient Alloy. United States. doi:10.1021/acsnano.7b06992.
Gao, Zhaoli, Zhang, Qicheng, Naylor, Carl H., Kim, Youngkuk, Abidi, Irfan Haider, Ping, Jinglei, Ducos, Pedro, Zauberman, Jonathan, Zhao, Meng -Qiang, Rappe, Andrew M., Luo, Zhengtang, Ren, Li, and Johnson, Alan T. Charlie. Tue . "Crystalline Bilayer Graphene with Preferential Stacking from Ni–Cu Gradient Alloy". United States. doi:10.1021/acsnano.7b06992. https://www.osti.gov/servlets/purl/1488924.
@article{osti_1488924,
title = {Crystalline Bilayer Graphene with Preferential Stacking from Ni–Cu Gradient Alloy},
author = {Gao, Zhaoli and Zhang, Qicheng and Naylor, Carl H. and Kim, Youngkuk and Abidi, Irfan Haider and Ping, Jinglei and Ducos, Pedro and Zauberman, Jonathan and Zhao, Meng -Qiang and Rappe, Andrew M. and Luo, Zhengtang and Ren, Li and Johnson, Alan T. Charlie},
abstractNote = {We developed a high-yield synthesis of highly crystalline bilayer graphene (BLG) with two preferential stacking modes using a Ni–Cu gradient alloy growth substrate. Previously reported approaches for BLG growth include flat growth substrates of Cu or Ni–Cu uniform alloys and “copper pocket” structures. Use of flat substrates has the advantage of being scalable, but the growth mechanism is either “surface limited” (for Cu) or carbon precipitation (for uniform Ni–Cu), which results in multicrystalline BLG grains. For copper pockets, growth proceeds through a carbon back-diffusion mechanism, which leads to the formation of highly crystalline BLG, but scaling of the copper pocket structure is expected to be difficult. Here we demonstrate a Ni–Cu gradient alloy that combines the advantages of these earlier methods: the substrate is flat, so easy to scale, while growth proceeds by a carbon back-diffusion mechanism leading to high-yield growth of BLG with high crystallinity. Here, the BLG layer stacking was almost exclusively Bernal or twisted with an angle of 30°, consistent with first-principles calculations we conducted. Furthermore, we demonstrated scalable production of transistor arrays based crystalline Bernal-stacked BLG with a band gap that was tunable at room temperature.},
doi = {10.1021/acsnano.7b06992},
journal = {ACS Nano},
number = 3,
volume = 12,
place = {United States},
year = {2018},
month = {3}
}

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