Scalable and ultrafast epitaxial growth of single-crystal graphene wafers for electrically tunable liquid-crystal microlens arrays.

The scalable growth of wafer-sized single-crystal graphene in an energy-efficient manner and compatible with wafer process is critical for the killer applications of graphene in high-performance electronics and optoelectronics. Here, ultrafast epitaxial growth of single-crystal graphene wafers is realized on single-crystal Cu90Ni10(1 1 1) thin films fabricated by a tailored two-step magnetron sputtering and recrystallization process. The minor nickel (Ni) content greatly enhances the catalytic activity of Cu, rendering the growth of a 4 in. single-crystal monolayer graphene wafer in 10 min on Cu90Ni10(1 1 1), 50 folds faster than graphene growth on Cu(1 1 1). Through the carbon isotope labeling experiments, graphene growth on Cu90Ni10(1 1 1) is proved to be exclusively surface-reaction dominated, which is ascribed to the Cu surface enrichment in the CuNi alloy, as indicated by element in-depth profile. One of the best benefits of our protocol is the compatibility with wafer process and excellent scalability. A pilot-scale chemical vapor deposition (CVD) system is designed and built for the mass production of single-crystal graphene wafers, with productivity of 25 pieces in one process cycle. Furthermore, we demonstrate the application of single-crystal graphene in electrically controlled liquid-crystal microlens arrays (LCMLA), which exhibit highly tunable focal lengths near 2 mm under small driving voltages. By integration of the graphene based LCMLA and a CMOS sensor, a prototype camera is proposed that is available for simultaneous light-field and light intensity imaging. The single-crystal graphene wafers could hold great promising for high-performance electronics and optoelectronics that are compatible with wafer process.

[1]  Hongwei Zhu,et al.  Synthesis of two dimensional materials on extremely clean surfaces , 2018, Nano Today.

[2]  Jing Zhao,et al.  Oxygen-Assisted Chemical Vapor Deposition Growth of Large Single-Crystal and High-Quality Monolayer MoS2. , 2015, Journal of the American Chemical Society.

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

[4]  Zhenyu Li,et al.  Gas-phase dynamics in graphene growth by chemical vapour deposition. , 2015, Physical chemistry chemical physics : PCCP.

[5]  M. Jiang,et al.  Fast growth of inch-sized single-crystalline graphene from a controlled single nucleus on Cu-Ni alloys. , 2016, Nature materials.

[6]  W. Guo,et al.  Controlling Fundamental Fluctuations for Reproducible Growth of Large Single-Crystal Graphene. , 2018, ACS nano.

[7]  C. Jin,et al.  Graphene annealing: how clean can it be? , 2012, Nano letters.

[8]  J. Tersoff,et al.  Structure and electronic transport in graphene wrinkles. , 2012, Nano letters.

[9]  Cheng Chen,et al.  Surface Monocrystallization of Copper Foil for Fast Growth of Large Single‐Crystal Graphene under Free Molecular Flow , 2016, Advanced materials.

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

[11]  Hee‐Tae Jung,et al.  Direct visualization of large-area graphene domains and boundaries by optical birefringency. , 2011, Nature nanotechnology.

[12]  K. Loh,et al.  Analyzing Dirac Cone and Phonon Dispersion in Highly Oriented Nanocrystalline Graphene. , 2016, ACS nano.

[13]  Yuduo Zhou,et al.  Fourier analysis of the focused plenoptic camera , 2013, Electronic Imaging.

[14]  R. Koch,et al.  Epitaxial Growth and Electronic Properties of Large Hexagonal Graphene Domains on Cu(111) Thin Film , 2013 .

[15]  P. Hanrahan,et al.  Light Field Photography with a Hand-held Plenoptic Camera , 2005 .

[16]  C. Gómez-Aleixandre,et al.  Review of CVD Synthesis of Graphene , 2013 .

[17]  Changsheng Xie,et al.  An electrically tunable plenoptic camera using a liquid crystal microlens array. , 2015, The Review of scientific instruments.

[18]  R. Ruoff,et al.  Ultrafast epitaxial growth of metre-sized single-crystal graphene on industrial Cu foil. , 2017, Science Bulletin.

[19]  Xiaohui Qiu,et al.  Wrinkle-Free Single-Crystal Graphene Wafer Grown on Strain-Engineered Substrates. , 2017, ACS nano.

[20]  H. Jeong,et al.  Wafer‐Scale Single‐Crystalline AB‐Stacked Bilayer Graphene , 2016, Advanced materials.

[21]  Luigi Colombo,et al.  Evolution of graphene growth on Ni and Cu by carbon isotope labeling. , 2009, Nano letters.

[22]  Kai Yan,et al.  Defect-like structures of graphene on copper foils for strain relief investigated by high-resolution scanning tunneling microscopy. , 2011, ACS nano.

[23]  I. Ford,et al.  Growth of Epitaxial Graphene: Theory and Experiment , 2014, 1602.06707.

[24]  F. Ding,et al.  How Low Nucleation Density of Graphene on CuNi Alloy is Achieved , 2018, Advanced science.

[25]  Andre K. Geim,et al.  Electric Field Effect in Atomically Thin Carbon Films , 2004, Science.

[26]  K. Novoselov,et al.  A roadmap for graphene , 2012, Nature.

[27]  B. Derby,et al.  Influence of gas phase equilibria on the chemical vapor deposition of graphene. , 2013, ACS nano.

[28]  A. Krasheninnikov,et al.  Structural defects in graphene. , 2011, ACS nano.

[29]  R. Ruoff,et al.  Synthesis of Graphene Films on Copper Foils by Chemical Vapor Deposition , 2016, Advances in Materials.

[30]  Bin Wang,et al.  Colossal grain growth yields single-crystal metal foils by contact-free annealing , 2018, Science.

[31]  Jingyu Sun,et al.  Rapid Growth of Large Single‐Crystalline Graphene via Second Passivation and Multistage Carbon Supply , 2016, Advanced materials.

[32]  K. Ikeda,et al.  Epitaxial growth of large-area single-layer graphene over Cu(111)/sapphire by atmospheric pressure CVD , 2012 .

[33]  K. Novoselov,et al.  Graphene-based liquid crystal device. , 2008, Nano letters (Print).

[34]  C. Xie,et al.  Dual-polarized light-field imaging micro-system via a liquid-crystal microlens array for direct three-dimensional observation. , 2018, Optics express.

[35]  F. Ding,et al.  The transition metal surface dependent methane decomposition in graphene chemical vapor deposition growth. , 2017, Nanoscale.

[36]  Enge Wang,et al.  Ultrafast growth of single-crystal graphene assisted by a continuous oxygen supply. , 2016, Nature nanotechnology.

[37]  Gunuk Wang,et al.  Large hexagonal bi- and trilayer graphene single crystals with varied interlayer rotations. , 2014, Angewandte Chemie.

[38]  Gwo-Ching Wang,et al.  Revealing the Crystalline Integrity of Wafer-Scale Graphene on SiO2/Si: An Azimuthal RHEED Approach. , 2017, ACS applied materials & interfaces.

[39]  N. Bartelt,et al.  Origin of the mosaicity in graphene grown on Cu(111) , 2011, 1107.1909.

[40]  Changsheng Xie,et al.  Dual-mode photosensitive arrays based on the integration of liquid crystal microlenses and CMOS sensors for obtaining the intensity images and wavefronts of objects. , 2016, Optics express.

[41]  Q. Fu,et al.  Heteroepitaxial growth of wafer scale highly oriented graphene using inductively coupled plasma chemical vapor deposition , 2016 .

[42]  Yi Cui,et al.  Roll-to-Roll Encapsulation of Metal Nanowires between Graphene and Plastic Substrate for High-Performance Flexible Transparent Electrodes. , 2015, Nano letters.

[43]  M. Keller,et al.  Epitaxial (111) Films of Cu, Ni, and Cu$_xNi$_y$ on {\alpha}-Al$_2$O$_3$(0001) for Graphene Growth by Chemical Vapor Deposition , 2012, 1205.0833.

[44]  Carl W. Magnuson,et al.  The Role of Surface Oxygen in the Growth of Large Single-Crystal Graphene on Copper , 2013, Science.

[45]  Philip D Rack,et al.  Evolutionary selection growth of two-dimensional materials on polycrystalline substrates , 2018, Nature Materials.

[46]  Edward B. Lochocki,et al.  Polycrystalline graphene with single crystalline electronic structure. , 2014, Nano letters.

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

[48]  Takashi Taniguchi,et al.  Epitaxial growth of single-domain graphene on hexagonal boron nitride. , 2013, Nature materials.

[49]  P. Chu,et al.  How Graphene Islands Are Unidirectionally Aligned on the Ge(110) Surface. , 2016, Nano letters.

[50]  Shuai Wang,et al.  Oxidative‐Etching‐Assisted Synthesis of Centimeter‐Sized Single‐Crystalline Graphene , 2016, Advanced materials.

[51]  J. Patel,et al.  Electrically controlled polarization-independent liquid-crystal Fresnel lens arrays. , 1991, Optics letters.

[52]  H Wang,et al.  Depth of field extension and objective space depth measurement based on wavefront imaging. , 2018, Optics express.

[53]  Eun Sung Kim,et al.  Probing graphene grain boundaries with optical microscopy , 2012, Nature.

[54]  Young Hee Lee,et al.  Towards Wafer-Scale Monocrystalline Graphene Growth and Characterization. , 2015, Small.

[55]  D. Ding,et al.  Spatially Controlled Nucleation of Single-Crystal Graphene on Cu Assisted by Stacked Ni. , 2016, ACS nano.

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

[57]  Byung-Sung Kim,et al.  Wafer-Scale Growth of Single-Crystal Monolayer Graphene on Reusable Hydrogen-Terminated Germanium , 2014, Science.

[58]  X. Duan,et al.  Chemical vapour deposition growth of large single crystals of monolayer and bilayer graphene , 2013, Nature Communications.

[59]  Ankanahalli Shankaregowda Smitha,et al.  Roll‐to‐Roll Green Transfer of CVD Graphene onto Plastic for a Transparent and Flexible Triboelectric Nanogenerator , 2015, Advanced materials.

[60]  A. Ferrari,et al.  Graphene Photonics and Optoelectroncs , 2010, CLEO 2012.

[61]  Zhongfan Liu,et al.  Graphene Glass Inducing Multidomain Orientations in Cholesteric Liquid Crystal Devices toward Wide Viewing Angles. , 2018, ACS nano.

[62]  Zhongfan Liu,et al.  Surface Engineering of Copper Foils for Growing Centimeter-Sized Single-Crystalline Graphene. , 2016, ACS Nano.

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

[64]  E. Tchernychova,et al.  Epitaxy and bonding of Cu films on oxygen-terminated α-Al2O3(0001) surfaces , 2006 .

[65]  G. A. Somorjai,et al.  THE SURFACE COMPOSITION OF BINARY SYSTEMS. PREDICTION OF SURFACE PHASE DIAGRAMS OF SOLID SOLUTIONS , 1975 .

[66]  Kai Yan,et al.  Designed CVD growth of graphene via process engineering. , 2013, Accounts of chemical research.