Self‐Assembly Growth of Twisted Bilayer Graphene on Liquid Cu

Twisted bilayer graphene (tBLG) possesses various novel physical properties. Most of tBLG are fabricated by using artificial methods of stacking or folding single‐layer graphene. Chemical vapor deposition (CVD) has been verified that it holds great potential for preparation of large‐size high‐quality graphene. Therefore, it is significant for preparing tBLG in situ by using CVD technology. In this work, a novel approach is developed to directly prepare tBLGs on liquid Cu substrate. When the growth temperature exceeds a certain critical value, the state of aligned high‐quality single‐layer graphene domains grown on liquid Cu will be broken. Then, tBLG with twisted double‐layer regions is prepared in situ by rotating and intercalating between graphene domains. Experimental observations suggest that the liquid phase of Cu substrate and gas flow play a crucial role for the formation of tBLGs. These results demonstrate that the liquid Cu is an ideal potential substrate for preparing tBLGs with a full range of twisted angles and studying the formation mechanism of layer‐stacked materials.

[1]  Yi Shi,et al.  Observation of chiral and slow plasmons in twisted bilayer graphene , 2022, Nature.

[2]  Liping Wang,et al.  Developing Graphene‐Based Moiré Heterostructures for Twistronics , 2021, Advanced science.

[3]  Kenji Watanabe,et al.  Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands , 2021, Nature Chemistry.

[4]  K. Novoselov,et al.  Hetero-site nucleation for growing twisted bilayer graphene with a wide range of twist angles , 2021, Nature Communications.

[5]  Qunyang Li,et al.  Abnormal conductivity in low-angle twisted bilayer graphene , 2020, Science Advances.

[6]  G. Qiao,et al.  Molecular dynamics simulation of graphene sinking during chemical vapor deposition growth on semi-molten Cu substrate , 2020, npj Computational Materials.

[7]  Bin Wang,et al.  Large-area single-crystal AB-bilayer and ABA-trilayer graphene grown on a Cu/Ni(111) foil , 2020, Nature Nanotechnology.

[8]  Birong Luo,et al.  Bilayer Graphene: From Stacking Order to Growth Mechanisms , 2020, physica status solidi (RRL) – Rapid Research Letters.

[9]  S. Du,et al.  Atomically precise, custom-design origami graphene nanostructures , 2019, Science.

[10]  Jie Yang,et al.  Design of carbon sources: starting point for chemical vapor deposition of graphene , 2019, 2D Materials.

[11]  Le Cai,et al.  Primary Nucleation-Dominated CVD Growth for Uniform Graphene Monolayers on Dielectric Substrate. , 2019, Journal of the American Chemical Society.

[12]  Hailong Zhu,et al.  Epitaxial Growth of 6 in. Single-Crystalline Graphene on a Cu/Ni (111) Film at 750 °C via Chemical Vapor Deposition. , 2019, Small.

[13]  T. Ma,et al.  Gas-Flow-Driven Aligned Growth of Graphene on Liquid Copper , 2019, Chemistry of Materials.

[14]  Zhongfan Liu,et al.  Toward Mass Production of CVD Graphene Films , 2018, Advanced materials.

[15]  Takashi Taniguchi,et al.  Unconventional superconductivity in magic-angle graphene superlattices , 2018, Nature.

[16]  E. Kaxiras,et al.  Correlated insulator behaviour at half-filling in magic-angle graphene superlattices , 2018, Nature.

[17]  Na Yeon Kim,et al.  Controlled Folding of Single Crystal Graphene. , 2017, Nano letters.

[18]  G. Yu,et al.  Etching-Controlled Growth of Graphene by Chemical Vapor Deposition , 2017 .

[19]  G. Yu,et al.  Direct CVD Graphene Growth on Semiconductors and Dielectrics for Transfer‐Free Device Fabrication , 2016, Advanced materials.

[20]  S. Okada,et al.  Highly Uniform Bilayer Graphene on Epitaxial Cu–Ni(111) Alloy , 2016 .

[21]  Jinxiong Wu,et al.  Building Large-Domain Twisted Bilayer Graphene with van Hove Singularity. , 2016, ACS nano.

[22]  R. Ruoff,et al.  Oxygen-activated growth and bandgap tunability of large single-crystal bilayer graphene. , 2016, Nature nanotechnology.

[23]  G. Yu,et al.  Graphene Single Crystals: Size and Morphology Engineering , 2015, Advanced materials.

[24]  Feng Ding,et al.  Seamless Stitching of Graphene Domains on Polished Copper (111) Foil , 2015, Advanced materials.

[25]  P. Chiu,et al.  Twisting bilayer graphene superlattices. , 2013, ACS nano.

[26]  X. Duan,et al.  High-yield chemical vapor deposition growth of high-quality large-area AB-stacked bilayer graphene. , 2012, ACS nano.

[27]  R. Hennig,et al.  Angle-resolved Raman imaging of interlayer rotations and interactions in twisted bilayer graphene. , 2012, Nano letters.

[28]  Liping Huang,et al.  Uniform hexagonal graphene flakes and films grown on liquid copper surface , 2012, Proceedings of the National Academy of Sciences.

[29]  Q. Fu,et al.  Repeated growth and bubbling transfer of graphene with millimetre-size single-crystal grains using platinum , 2012, Nature Communications.

[30]  K. Loh,et al.  Electrochemical delamination of CVD-grown graphene film: toward the recyclable use of copper catalyst. , 2011, ACS nano.

[31]  Yanfeng Zhang,et al.  Single-layer behavior and slow carrier density dynamic of twisted graphene bilayer , 2011, 1111.0411.

[32]  R. Ruoff,et al.  Graphene and Graphene Oxide: Synthesis, Properties, and Applications , 2010, Advanced materials.

[33]  Marc J. Assael,et al.  Reference Data for the Density and Viscosity of Liquid Copper and Liquid Tin , 2010 .

[34]  Eun Sung Kim,et al.  Synthesis of Large‐Area Graphene Layers on Poly‐Nickel Substrate by Chemical Vapor Deposition: Wrinkle Formation , 2009 .

[35]  D. Mayou,et al.  Localization of dirac electrons in rotated graphene bilayers. , 2009, Nano letters.

[36]  Zhenhua Ni,et al.  Raman Mapping Investigation of Graphene on Transparent Flexible Substrate: The Strain Effect , 2008 .

[37]  A. Neto,et al.  Making graphene visible , 2007, Applied Physics Letters.