Large hexagonal bi- and trilayer graphene single crystals with varied interlayer rotations.

Bi- and trilayer graphene have attracted intensive interest due to their rich electronic and optical properties, which are dependent on interlayer rotations. However, the synthesis of high-quality large-size bi- and trilayer graphene single crystals still remains a challenge. Here, the synthesis of 100 μm pyramid-like hexagonal bi- and trilayer graphene single-crystal domains on Cu foils using chemical vapor deposition is reported. The as-produced graphene domains show almost exclusively either 0° or 30° interlayer rotations. Raman spectroscopy, transmission electron microscopy, and Fourier-transformed infrared spectroscopy were used to demonstrate that bilayer graphene domains with 0° interlayer stacking angles were Bernal stacked. Based on first-principle calculations, it is proposed that rotations originate from the graphene nucleation at the Cu step, which explains the origin of the interlayer rotations and agrees well with the experimental observations.

[1]  J. Kong,et al.  Rapid identification of stacking orientation in isotopically labeled chemical-vapor grown bilayer graphene by Raman spectroscopy. , 2013, Nano letters.

[2]  Ting Yu,et al.  Terahertz conductivity of twisted bilayer graphene. , 2013, Physical review letters.

[3]  J. Xin,et al.  How the Orientation of Graphene Is Determined during Chemical Vapor Deposition Growth , 2012 .

[4]  J. Tour,et al.  Toward the synthesis of wafer-scale single-crystal graphene on copper foils. , 2012, ACS nano.

[5]  B. Yakobson,et al.  Equilibrium at the edge and atomistic mechanisms of graphene growth , 2012, Proceedings of the National Academy of Sciences.

[6]  Sang Wook Lee,et al.  Breakdown of the interlayer coherence in twisted bilayer graphene. , 2012, Physical review letters.

[7]  S. Louie,et al.  Raman spectroscopy study of rotated double-layer graphene: misorientation-angle dependence of electronic structure. , 2012, Physical review letters.

[8]  Eun Sung Kim,et al.  Influence of copper morphology in forming nucleation seeds for graphene growth. , 2011, Nano letters.

[9]  Y. Shibuta,et al.  Interaction between two graphene sheets with a turbostratic orientational relationship , 2011 .

[10]  Yan Zhang,et al.  The experimental observation of quantum Hall effect of lD3 chiral quasiparticles in trilayer graphene , 2011, 1103.6023.

[11]  Jijun Zhao,et al.  Graphene nucleation on transition metal surface: structure transformation and role of the metal step edge. , 2011, Journal of the American Chemical Society.

[12]  Hui Li,et al.  Formation of bilayer bernal graphene: layer-by-layer epitaxy via chemical vapor deposition. , 2011, Nano letters.

[13]  Luigi Colombo,et al.  Large-area graphene single crystals grown by low-pressure chemical vapor deposition of methane on copper. , 2011, Journal of the American Chemical Society.

[14]  S. Pei,et al.  Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition. , 2010, Nature materials.

[15]  Z. Zhong,et al.  Wafer scale homogeneous bilayer graphene films by chemical vapor deposition. , 2010, Nano letters.

[16]  Pinshane Y. Huang,et al.  Grains and grain boundaries in single-layer graphene atomic patchwork quilts , 2010, Nature.

[17]  B. Yakobson,et al.  Graphene edge from armchair to zigzag: the origins of nanotube chirality? , 2010, Physical review letters.

[18]  N. Guisinger,et al.  Epitaxial graphene on Cu(111). , 2010, Nano letters.

[19]  J. Nørskov,et al.  On the Role of Metal Step-Edges in Graphene Growth , 2010 .

[20]  D. Shen,et al.  Stacking-dependent optical conductivity of bilayer graphene. , 2010, ACS nano.

[21]  A. Reina,et al.  Large area, few-layer graphene films on arbitrary substrates by chemical vapor deposition. , 2009, Nano letters.

[22]  T. Tang,et al.  Direct observation of a widely tunable bandgap in bilayer graphene , 2009, Nature.

[23]  S. Banerjee,et al.  Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils , 2009, Science.

[24]  M. Dresselhaus,et al.  Raman spectroscopy in graphene , 2009 .

[25]  Kwang S. Kim,et al.  Large-scale pattern growth of graphene films for stretchable transparent electrodes , 2009, Nature.

[26]  J. Coleman,et al.  High-yield production of graphene by liquid-phase exfoliation of graphite. , 2008, Nature nanotechnology.

[27]  Feng Wang,et al.  Gate-Variable Optical Transitions in Graphene , 2008, Science.

[28]  G. Fudenberg,et al.  Ultrahigh electron mobility in suspended graphene , 2008, 0802.2389.

[29]  Andre K. Geim,et al.  The rise of graphene. , 2007, Nature materials.

[30]  D. Warrington.  THE COINCIDENCE SITE LATTICE (CSL) AND GRAIN BOUNDARY (DSC) DISLOCATIONS FOR THE HEXAGONAL LATTICE , 1975 .