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Title: Fabrication of Millimeter-Scale, Single-Crystal One-Third-Hydrogenated Graphene with Anisotropic Electronic Properties

Abstract

Abstract Periodically hydrogenated graphene is predicted to form new kinds of crystalline 2D materials such as graphane, graphone, and 2D C x H y , which exhibit unique electronic properties. Controlled synthesis of periodically hydrogenated graphene is needed for fundamental research and possible electronic applications. Only small patches of such materials have been grown so far, while the experimental fabrication of large‐scale, periodically hydrogenated graphene has remained challenging. In the present work, large‐scale, periodically hydrogenated graphene is fabricated on Ru(0001). The as‐fabricated hydrogenated graphene is highly ordered, with a √3 × √3/R30° period relative to the pristine graphene. As the ratio of hydrogen and carbon is 1:3, the periodically hydrogenated graphene is named “one‐third‐hydrogenated graphene” (OTHG). The area of OTHG is up to 16 mm 2 . Density functional theory calculations demonstrate that the OTHG has two deformed Dirac cones along one high‐symmetry direction and a finite energy gap along the other directions at the Fermi energy, indicating strong anisotropic electrical properties. An efficient method is thus provided to produce large‐scale crystalline functionalized graphene with specially desired properties.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1];  [2];  [1]
  1. University of Chinese Academy of Sciences, Beijing (China)
  2. University of Chinese Academy of Sciences, Beijing (China); Vanderbilt University, Nashville, TN (United States)
Publication Date:
Research Org.:
Vanderbilt Univ., Nashville, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Natural Science Foundation of China (NSFC); National Key Research and Development Projects of China; Chinese Academy of Sciences (CAS); Beijing Nova Program
OSTI Identifier:
1597905
Alternate Identifier(s):
OSTI ID: 1457064
Grant/Contract Number:  
FG02-09ER46554; 61390501; 51761135130; 2016YFA0202300; 2016YFA0300904; XDPB0601; XDB07030100; XDPB08-1; Z181100006218023; AC02-05CH11231; DE‐FG02‐09ER46554; DE‐AC02‐05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 32; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; anisotropy; hydrogenated graphene; millimeter-scale; single crystals

Citation Formats

Chen, Hui, Bao, De-Liang, Wang, Dongfei, Que, Yande, Xiao, Wende, Qian, Guojian, Guo, Hui, Sun, Jiatao, Zhang, Yu-Yang, Du, Shixuan, Pantelides, Sokrates T., and Gao, Hong-Jun. Fabrication of Millimeter-Scale, Single-Crystal One-Third-Hydrogenated Graphene with Anisotropic Electronic Properties. United States: N. p., 2018. Web. doi:10.1002/adma.201801838.
Chen, Hui, Bao, De-Liang, Wang, Dongfei, Que, Yande, Xiao, Wende, Qian, Guojian, Guo, Hui, Sun, Jiatao, Zhang, Yu-Yang, Du, Shixuan, Pantelides, Sokrates T., & Gao, Hong-Jun. Fabrication of Millimeter-Scale, Single-Crystal One-Third-Hydrogenated Graphene with Anisotropic Electronic Properties. United States. https://doi.org/10.1002/adma.201801838
Chen, Hui, Bao, De-Liang, Wang, Dongfei, Que, Yande, Xiao, Wende, Qian, Guojian, Guo, Hui, Sun, Jiatao, Zhang, Yu-Yang, Du, Shixuan, Pantelides, Sokrates T., and Gao, Hong-Jun. Mon . "Fabrication of Millimeter-Scale, Single-Crystal One-Third-Hydrogenated Graphene with Anisotropic Electronic Properties". United States. https://doi.org/10.1002/adma.201801838. https://www.osti.gov/servlets/purl/1597905.
@article{osti_1597905,
title = {Fabrication of Millimeter-Scale, Single-Crystal One-Third-Hydrogenated Graphene with Anisotropic Electronic Properties},
author = {Chen, Hui and Bao, De-Liang and Wang, Dongfei and Que, Yande and Xiao, Wende and Qian, Guojian and Guo, Hui and Sun, Jiatao and Zhang, Yu-Yang and Du, Shixuan and Pantelides, Sokrates T. and Gao, Hong-Jun},
abstractNote = {Abstract Periodically hydrogenated graphene is predicted to form new kinds of crystalline 2D materials such as graphane, graphone, and 2D C x H y , which exhibit unique electronic properties. Controlled synthesis of periodically hydrogenated graphene is needed for fundamental research and possible electronic applications. Only small patches of such materials have been grown so far, while the experimental fabrication of large‐scale, periodically hydrogenated graphene has remained challenging. In the present work, large‐scale, periodically hydrogenated graphene is fabricated on Ru(0001). The as‐fabricated hydrogenated graphene is highly ordered, with a √3 × √3/R30° period relative to the pristine graphene. As the ratio of hydrogen and carbon is 1:3, the periodically hydrogenated graphene is named “one‐third‐hydrogenated graphene” (OTHG). The area of OTHG is up to 16 mm 2 . Density functional theory calculations demonstrate that the OTHG has two deformed Dirac cones along one high‐symmetry direction and a finite energy gap along the other directions at the Fermi energy, indicating strong anisotropic electrical properties. An efficient method is thus provided to produce large‐scale crystalline functionalized graphene with specially desired properties.},
doi = {10.1002/adma.201801838},
journal = {Advanced Materials},
number = 32,
volume = 30,
place = {United States},
year = {Mon Jun 25 00:00:00 EDT 2018},
month = {Mon Jun 25 00:00:00 EDT 2018}
}

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Cited by: 27 works
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Figures / Tables:

Figure 1 Figure 1: Large-scale synthesis of periodically-hydrogenated graphene on Ru(0001). a) Schematic showing the fabrication of periodically-hydrogenated graphene on Ru(0001) through atomic hydrogen chemisorption. b) LEED pattern of graphene (left panel) and hydrogenated graphene (right panel) on Ru(0001). The red and yellow arrows indicate the diffraction spots from graphene and Ru(0001),more » respectively. The white circles indicate the √3 × √3/R30° with respect to graphene induced by hydrogenation. The beam energy is 69 eV. (c) A large-scale STM image of hydrogenated graphene on Ru(0001) and corresponding fast Fourier transformation (FFT) of the image (inset), showing the formation of hexagonal patterns (Sample bias: U = -20 mV, Tunneling current: I = 0.2 nA). (d) Raman spectra of graphene (red curve) and periodically-hydrogenated graphene (black curve) on Ru(0001), showing the recovery of the G peak and 2D peak. The inset shows a high-resolution spectrum of the G and D′ band of hydrogenated graphene.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.