Controlling Water Intercalation Is Key to a Direct Graphene Transfer.

The key steps of a transfer of two-dimensional (2D) materials are the delamination of the as-grown material from a growth substrate and the lamination of the 2D material on a target substrate. In state-of-the-art transfer experiments, these steps remain very challenging, and transfer variations often result in unreliable 2D material properties. Here, it is demonstrated that interfacial water can insert between graphene and its growth substrate despite the hydrophobic behavior of graphene. It is understood that interfacial water is essential for an electrochemistry-based graphene delamination from a Pt surface. Additionally, the lamination of graphene to a target wafer is hindered by intercalation effects, which can even result in graphene delamination from the target wafer. For circumvention of these issues, a direct, support-free graphene transfer process is demonstrated, which relies on the formation of interfacial water between graphene and its growth surface, while avoiding water intercalation between graphene and the target wafer by using hydrophobic silane layers on the target wafer. The proposed direct graphene transfer also avoids polymer contamination (no temporary support layer) and eliminates the need for etching of the catalyst metal. Therefore, recycling of the growth template becomes feasible. The proposed transfer process might even open the door for the suggested atomic-scale interlocking-toy-brick-based stacking of different 2D materials, which will enable a more reliable fabrication of van der Waals heterostructure-based devices and applications.

[1]  M. Dresselhaus,et al.  Studying disorder in graphite-based systems by Raman spectroscopy. , 2007, Physical chemistry chemical physics : PCCP.

[2]  P. Blaha,et al.  Calculation of the lattice constant of solids with semilocal functionals , 2009 .

[3]  Xu Xie,et al.  Controlled fabrication of high-quality carbon nanoscrolls from monolayer graphene. , 2009, Nano letters.

[4]  Xiaojun Weng,et al.  Correlating Raman spectral signatures with carrier mobility in epitaxial graphene: a guide to achieving high mobility on the wafer scale. , 2009, Nano letters.

[5]  John A. Rogers,et al.  Transfer of graphene layers grown on SiC wafers to other substrates and their integration into field effect transistors , 2009 .

[6]  J. Heath,et al.  Graphene Visualizes the First Water Adlayers on Mica at Ambient Conditions , 2010, Science.

[7]  L. Vandersypen,et al.  Wedging transfer of nanostructures. , 2010, Nano letters.

[8]  Zhiping Xu,et al.  Geometry controls conformation of graphene sheets: membranes, ribbons, and scrolls. , 2010, ACS nano.

[9]  James M Tour,et al.  Controlled modulation of electronic properties of graphene by self-assembled monolayers on SiO2 substrates. , 2011, ACS nano.

[10]  Electrical transport properties of graphene on SiO2 with specific surface structures , 2011, 1106.5813.

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

[12]  T. Michely,et al.  Interplay of wrinkles, strain, and lattice parameter in graphene on iridium. , 2012, Nano letters.

[13]  Niclas Lindvall,et al.  Determination of the bending rigidity of graphene via electrostatic actuation of buckled membranes. , 2012, Nano letters.

[14]  Eric Pop,et al.  Scanning tunneling microscopy study and nanomanipulation of graphene-coated water on mica. , 2012, Nano letters.

[15]  Jan Szmidt,et al.  Properties of Chemical Vapor Deposition Graphene Transferred by High-Speed Electrochemical Delamination , 2013 .

[16]  Hui‐Ming Cheng,et al.  Edge-controlled growth and kinetics of single-crystal graphene domains by chemical vapor deposition , 2013, Proceedings of the National Academy of Sciences.

[17]  SUPARNA DUTTASINHA,et al.  Van der Waals heterostructures , 2013, Nature.

[18]  M. Cole,et al.  Frame assisted H2O electrolysis induced H2 bubbling transfer of large area graphene grown by chemical vapor deposition on Cu , 2013 .

[19]  Lianmao Peng,et al.  How good can CVD-grown monolayer graphene be? , 2014, Nanoscale.

[20]  Jan-Kai Chang,et al.  A direct and polymer-free method for transferring graphene grown by chemical vapor deposition to any substrate. , 2014, ACS nano.

[21]  Takashi Taniguchi,et al.  Random Strain Fluctuations as Dominant Disorder Source for High-Quality On-Substrate Graphene Devices , 2014, 1401.5356.

[22]  O. Ochedowski,et al.  Graphene on Mica - Intercalated Water Trapped for Life , 2014, Scientific Reports.

[23]  S. Louie,et al.  The imprint of transition metal d-orbitals on a graphene Dirac cone: A Raman investigation , 2014 .

[24]  S. Ryu,et al.  Two-dimensional water diffusion at a graphene-silica interface. , 2014, Journal of the American Chemical Society.

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

[26]  Joon Young Kwak,et al.  A universal transfer route for graphene. , 2014, Nanoscale.

[27]  Shanshan Yao,et al.  Surface-energy-assisted perfect transfer of centimeter-scale monolayer and few-layer MoS₂ films onto arbitrary substrates. , 2014, ACS nano.

[28]  K. Loh,et al.  Face-to-face transfer of wafer-scale graphene films , 2013, Nature.

[29]  P. Bøggild,et al.  Facile electrochemical transfer of large-area single crystal epitaxial graphene from Ir(1 1 1) , 2015 .

[30]  Latent heat induced rotation limited aggregation in 2D ice nanocrystals. , 2015, The Journal of chemical physics.

[31]  C. Stampfer,et al.  Raman spectroscopy as probe of nanometre-scale strain variations in graphene , 2014, Nature Communications.

[32]  Jianbo Yin,et al.  A universal etching-free transfer of MoS2 films for applications in photodetectors , 2015, Nano Research.

[33]  S. Kang,et al.  Growth of wrinkle-free graphene on texture-controlled platinum films and thermal-assisted transfer of large-scale patterned graphene. , 2015, ACS nano.

[34]  N. Grobert,et al.  Rapid epitaxy-free graphene synthesis on silicidated polycrystalline platinum , 2015, Nature Communications.

[35]  A. Oral,et al.  Synthesis of few layer single crystal graphene grains on platinum by chemical vapour deposition , 2015 .

[36]  Sung‐Yool Choi,et al.  Metal-etching-free direct delamination and transfer of single-layer graphene with a high degree of freedom. , 2015, Small.

[37]  C. Stampfer,et al.  Ultrahigh-mobility graphene devices from chemical vapor deposition on reusable copper , 2015, Science Advances.

[38]  Mikael Östling,et al.  Residual metallic contamination of transferred chemical vapor deposited graphene. , 2015, ACS nano.

[39]  B. Özyilmaz,et al.  'Bubble-free' electrochemical delamination of CVD graphene films. , 2015, Small.

[40]  D. Lohse,et al.  Structure and Dynamics of Confined Alcohol-Water Mixtures. , 2016, ACS nano.

[41]  K. Cho,et al.  Wetting‐Assisted Crack‐ and Wrinkle‐Free Transfer of Wafer‐Scale Graphene onto Arbitrary Substrates over a Wide Range of Surface Energies , 2016 .

[42]  M. Willinger,et al.  In Situ Graphene Growth Dynamics on Polycrystalline Catalyst Foils , 2016, Nano letters.

[43]  Fernando Calle,et al.  Automatic graphene transfer system for improved material quality and efficiency , 2016, Scientific Reports.

[44]  A. Oral,et al.  Suitable alkaline for graphene peeling grown on metallic catalysts using chemical vapor deposition , 2016 .

[45]  J. Shappir,et al.  On-Chip Integrated, Silicon–Graphene Plasmonic Schottky Photodetector with High Responsivity and Avalanche Photogain , 2015, Nano letters.

[46]  Xing Fan,et al.  Electrochemical Bubbling Transfer of Graphene Using a Polymer Support with Encapsulated Air Gap as Permeation Stopping Layer , 2016 .

[47]  Electroinduced Intercalation of Tetraalkylammonium Ions at the Interface of Graphene Grown on Copper, Platinum, and Iridium , 2016 .

[48]  R. Ruoff,et al.  Support-Free Transfer of Ultrasmooth Graphene Films Facilitated by Self-Assembled Monolayers for Electronic Devices and Patterns. , 2016, ACS nano.

[49]  M. Righi,et al.  Graphene and MoS2 interacting with water: A comparison by ab initio calculations , 2016, 1607.05607.

[50]  V. Tsukruk,et al.  Ultrastrong Freestanding Graphene Oxide Nanomembranes with Surface-Enhanced Raman Scattering Functionality by Solvent-Assisted Single-Component Layer-by-Layer Assembly. , 2016, ACS nano.

[51]  S. Koh,et al.  Epitaxial growth and electrochemical transfer of graphene on Ir(111)/α-Al2O3(0001) substrates , 2016 .

[52]  B. Poelsema,et al.  Electrochemically Induced Nanobubbles between Graphene and Mica. , 2016, Langmuir : the ACS journal of surfaces and colloids.