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

Journal Article · · Nature Nanotechnology

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.

Research Organization:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
DOE Contract Number:
AC36-08GO28308
OSTI ID:
1253273
Report Number(s):
NREL/JA-5K00-65891; MainId:12287; UUID:0e574a12-78cf-e511-97db-d89d67132a6d; MainAdminID:767
Journal Information:
Nature Nanotechnology, Vol. 11, Issue 5; Related Information: Nature Nanotechnology; ISSN 1748-3387
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English

References (30)

The rise of graphene journal March 2007
Direct observation of a widely tunable bandgap in bilayer graphene journal June 2009
Dual-gated bilayer graphene hot-electron bolometer journal June 2012
Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition journal May 2011
Electronic transport in polycrystalline graphene journal August 2010
Raman Spectroscopy Study of Rotated Double-Layer Graphene: Misorientation-Angle Dependence of Electronic Structure journal June 2012
The surface science of graphene: Metal interfaces, CVD synthesis, nanoribbons, chemical modifications, and defects journal March 2012
Large-scale pattern growth of graphene films for stretchable transparent electrodes journal January 2009
Interdependency of Subsurface Carbon Distribution and Graphene–Catalyst Interaction journal September 2014
A review of chemical vapour deposition of graphene on copper journal January 2011
Wafer Scale Homogeneous Bilayer Graphene Films by Chemical Vapor Deposition journal November 2010
Controllable and Rapid Synthesis of High-Quality and Large-Area Bernal Stacked Bilayer Graphene Using Chemical Vapor Deposition journal December 2013
Chemical vapour deposition growth of large single crystals of monolayer and bilayer graphene journal June 2013
Formation of Bilayer Bernal Graphene: Layer-by-Layer Epitaxy via Chemical Vapor Deposition journal March 2011
Asymmetric Growth of Bilayer Graphene on Copper Enclosures Using Low-Pressure Chemical Vapor Deposition journal May 2014
Large-Area Bernal-Stacked Bi-, Tri-, and Tetralayer Graphene journal October 2012
High-Yield Chemical Vapor Deposition Growth of High-Quality Large-Area AB-Stacked Bilayer Graphene journal August 2012
Equilibrium Chemical Vapor Deposition Growth of Bernal-Stacked Bilayer Graphene journal November 2014
The Role of Surface Oxygen in the Growth of Large Single-Crystal Graphene on Copper journal October 2013
Probing Layer Number and Stacking Order of Few-Layer Graphene by Raman Spectroscopy journal January 2010
Graphene Nucleation Density on Copper: Fundamental Role of Background Pressure journal September 2013
Toward the Synthesis of Wafer-Scale Single-Crystal Graphene on Copper Foils journal September 2012
Evolution of Graphene Growth on Ni and Cu by Carbon Isotope Labeling journal December 2009
Activation Energy Paths for Graphene Nucleation and Growth on Cu journal March 2012
The solubility of C in solid Cu journal July 2004
Observing Graphene Grow: Catalyst–Graphene Interactions during Scalable Graphene Growth on Polycrystalline Copper journal September 2013
The Role of Stable and Mobile Carbon Adspecies in Copper-Promoted Graphene Growth journal February 2012
First-Principles Thermodynamics of Graphene Growth on Cu Surfaces journal August 2011
Electronic Transport in Dual-Gated Bilayer Graphene at Large Displacement Fields journal October 2010
Rapid Identification of Stacking Orientation in Isotopically Labeled Chemical-Vapor Grown Bilayer Graphene by Raman Spectroscopy journal March 2013