Evolution of Electrical, Chemical, and Structural Properties of Transparent and Conducting Chemically Derived Graphene Thin Films

A detailed description of the electronic properties, chemical state, and structure of uniform single and few-layered graphene oxide (GO) thin films at different stages of reduction is reported. The residual oxygen content and structure of GO are monitored and these chemical and structural characteristics are correlated to electronic properties of the thin films at various stages of reduction. It is found that the electrical characteristics of reduced GO do not approach those of intrinsic graphene obtained by mechanical cleaving because the material remains significantly oxidized. The residual oxygen forms sp3 bonds with carbon atoms in the basal plane such that the carbon sp2 bonding fraction in fully reduced GO is ∼0.80. The minority sp3 bonds disrupt the transport of carriers delocalized in the sp2 network, limiting the mobility, and conductivity of reduced GO thin films. Extrapolation of electrical conductivity data as a function of oxygen content reveals that complete removal of oxygen should lead to properties that are comparable to graphene.

[1]  P. Kim,et al.  Experimental observation of the quantum Hall effect and Berry's phase in graphene , 2005, Nature.

[2]  Inhwa Jung,et al.  Tunable electrical conductivity of individual graphene oxide sheets reduced at "low" temperatures. , 2008, Nano letters.

[3]  S. Stankovich,et al.  Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and Micro-Raman spectroscopy , 2009 .

[4]  Kang L. Wang,et al.  A chemical route to graphene for device applications. , 2007, Nano letters.

[5]  Jacek Klinowski,et al.  A new structural model for graphite oxide , 1998 .

[6]  J. Robinson,et al.  Wafer-scale reduced graphene oxide films for nanomechanical devices. , 2008, Nano letters.

[7]  Dongmin Chen,et al.  Synthesis and Solid-State NMR Structural Characterization of 13C-Labeled Graphite Oxide , 2008, Science.

[8]  F. Tuinstra,et al.  Raman Spectrum of Graphite , 1970 .

[9]  I. Balberg,et al.  Limits on the continuum-percolation transport exponents , 1998 .

[10]  Yang Yang,et al.  High-throughput solution processing of large-scale graphene. , 2009, Nature nanotechnology.

[11]  J. D. Lopez-Gonzalez,et al.  Study of oxygen-containing groups in a series of graphite oxides: Physical and chemical characterization , 1995 .

[12]  A. Geim,et al.  Two-dimensional gas of massless Dirac fermions in graphene , 2005, Nature.

[13]  P. T. Lillehei,et al.  AC and DC percolative conductivity of single wall carbon nanotube polymer composites , 2005 .

[14]  M I Katsnelson,et al.  Modeling of graphite oxide. , 2008, Journal of the American Chemical Society.

[15]  S. Marchini,et al.  Scanning tunneling microscopy of graphene on Ru(0001) , 2007 .

[16]  F. Banhart,et al.  Irradiation effects in carbon nanostructures , 1999 .

[17]  G. Amaratunga,et al.  Evolution of sp2 bonding with deposition temperature in tetrahedral amorphous carbon studied by Raman spectroscopy , 2000 .

[18]  J. Robertson,et al.  Raman spectroscopy of amorphous, nanostructured, diamond–like carbon, and nanodiamond , 2004, Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences.

[19]  S. Chou,et al.  Graphene transistors fabricated via transfer-printing in device active-areas on large wafer , 2007 .

[20]  Imre Dékány,et al.  Evolution of surface functional groups in a series of progressively oxidized graphite oxides , 2006 .

[21]  H. Dai,et al.  Highly conducting graphene sheets and Langmuir-Blodgett films. , 2008, Nature nanotechnology.

[22]  C. Berger,et al.  Electronic Confinement and Coherence in Patterned Epitaxial Graphene , 2006, Science.

[23]  S. Stankovich,et al.  Graphene-based composite materials , 2006, Nature.

[24]  Xu Du,et al.  Approaching ballistic transport in suspended graphene. , 2008, Nature nanotechnology.

[25]  宁北芳,et al.  疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A , 2005 .

[26]  G. Eda,et al.  Large-area ultrathin films of reduced graphene oxide as a transparent and flexible electronic material. , 2008, Nature nanotechnology.

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

[28]  A. V. Fedorov,et al.  Substrate-induced bandgap opening in epitaxial graphene. , 2007, Nature materials.

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

[30]  Edward Sacher,et al.  Carbon 1s X-ray photoemission line shape analysis of highly oriented pyrolytic graphite: the influence of structural damage on peak asymmetry. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[31]  Zhaobo Wang,et al.  Ni-Fe-Co-P coatings on coiled carbon nanofibers , 2005 .

[32]  N. Balzaretti,et al.  High pressure annealing of defects induced by ion implantation on graphite , 2001 .

[33]  E. Samulski,et al.  Synthesis of water soluble graphene. , 2008, Nano letters.

[34]  C. H. Seager,et al.  Percolation and conductivity: A computer study. II , 1974 .

[35]  R. Rosenfeld.  Nature , 2009, Otolaryngology--head and neck surgery : official journal of American Academy of Otolaryngology-Head and Neck Surgery.

[36]  R. Stoltenberg,et al.  Evaluation of solution-processed reduced graphene oxide films as transparent conductors. , 2008, ACS nano.

[37]  G. Wallace,et al.  Processable aqueous dispersions of graphene nanosheets. , 2008, Nature nanotechnology.

[38]  Klaus Kern,et al.  Electronic transport properties of individual chemically reduced graphene oxide sheets. , 2007, Nano letters.

[39]  D. R. Penn,et al.  Calculations of electron inelastic mean free paths. III. Data for 15 inorganic compounds over the 50–2000 eV range , 1991 .

[40]  S. Stankovich,et al.  Synthesis of graphene-based nanosheets via chemical reduction of exfoliated graphite oxide , 2007 .

[41]  T. Belytschko,et al.  Computational Studies of the Structure, Behavior upon Heating, and Mechanical Properties of Graphite Oxide , 2007 .

[42]  Jacek Klinowski,et al.  Structure of Graphite Oxide Revisited , 1998 .

[43]  Yan Jie Li,et al.  Investigation on the Deformation of TiNi Shape Memory Alloy with a Crack Using Moiré Interferometry , 2008 .

[44]  John Silcox,et al.  Atomic and electronic structure of graphene-oxide. , 2009, Nano letters.