First-principles studies of water adsorption on graphene: The role of the substrate

We investigate the electronic properties of graphene upon water adsorption and study the influence of the SiO2 substrate in this context using density functional calculations. Perfect suspended graphene is rather insensitive to H2O adsorbates, as doping requires highly oriented H2O clusters. For graphene on a defective SiO2 substrate, we find a strongly different behavior: H2O adsorbates can shift the substrate’s impurity bands and change their hybridization with the graphene bands. In this way, H2O can lead to doping of graphene for much lower adsorbate concentrations than for free hanged graphene. The effect depends strongly on the microscopic substrate properties.

[1]  G. Kresse,et al.  From ultrasoft pseudopotentials to the projector augmented-wave method , 1999 .

[2]  Patricia A. Thiel,et al.  The interaction of water with solid surfaces: Fundamental aspects , 1987 .

[3]  Jijun Zhao,et al.  Gas molecule adsorption in carbon nanotubes and nanotube bundles , 2002 .

[4]  A. Bachtold,et al.  The environment of graphene probed by electrostatic force microscopy , 2008, 0803.2032.

[5]  E. Kaxiras,et al.  Water wettability of close-packed metal surfaces. , 2007, The Journal of chemical physics.

[6]  F. M. Peeters,et al.  Adsorption of H 2 O , N H 3 , CO, N O 2 , and NO on graphene: A first-principles study , 2007, 0710.1757.

[7]  Blöchl,et al.  Projector augmented-wave method. , 1994, Physical review. B, Condensed matter.

[8]  L. Oroszlány,et al.  Adsorbate-limited conductivity of graphene. , 2008, Physical review letters.

[9]  K. Novoselov,et al.  Molecular doping of graphene. , 2007, Nano letters.

[10]  G. G. Stokes.  "J." , 1890, The New Yale Book of Quotations.

[11]  Jackson,et al.  Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation. , 1992, Physical review. B, Condensed matter.

[12]  Andre K. Geim,et al.  Two-dimensional atomic crystals. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[13]  A graphene-based electrochemical switch , 2007, 0712.2026.

[14]  Burke,et al.  Generalized Gradient Approximation Made Simple. , 1996, Physical review letters.

[15]  Georg Kresse,et al.  Norm-conserving and ultrasoft pseudopotentials for first-row and transition elements , 1994 .

[16]  Ophir Vermesh,et al.  Hysteresis caused by water molecules in carbon nanotube field-effect transistors , 2003 .

[17]  K. Novoselov,et al.  Giant intrinsic carrier mobilities in graphene and its bilayer. , 2007, Physical review letters.

[18]  Andrew G. Glen,et al.  APPL , 2001 .

[19]  N. Peres,et al.  Inducing energy gaps in monolayer and bilayer graphene: Local density approximation calculations , 2008 .

[20]  A. Wright,et al.  The structures of the β-cristobalite phases of SiO2 and AlPO4 , 1975 .

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

[22]  T. Walsh,et al.  Hydrolysis of the amorphous silica surface. I. Structure and dynamics of the dry surface , 2000 .

[23]  K. Novoselov,et al.  Detection of individual gas molecules adsorbed on graphene. , 2006, Nature materials.

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

[25]  F. Guinea,et al.  Electrostatic interactions between graphene layers and their environment , 2007, 0712.2232.