Results of room temperature Raman scattering studies of ultrathin graphitic films supported on Si (111)/SiO 2 substrates are reported. The results are significantly different from those known for graphite. Spectra were collected using 514 nm radiation on films containing from n=1 to 20 graphene layers, as determined by atomic force microscopy. Both the 1 st and 2 nd order Raman spectra show unique signatures of the number of layers in the film. The nGL film analog of the Raman G-band in graphite exhibits a Lorentzian lineshape whose center frequency shifts linearly relative to graphite as ~1/n (for n=1 ω G~1 588 cm -1 ). Three weak bands, identified with disorder-induced 1 st order scattering, are observed at ~ 1350, 1450 and 1500 cm -1 . The 1500 cm -1 band is weak but relatively sharp and exhibits an interesting n-dependence. In general, the intensity of these D-bands decreases dramatically with increasing n. Three 2 nd order bands are also observed (~2450, ~2700 and 3248 cm -1 ). They are analogs to those observed in graphite. However, the ~2700 cm -1 band exhibits an interesting and dramatic change of shape with n. Interestingly, for n<5 this 2 nd order band is more intense than the G-band.

Results are presented from an experimental and theoretical study of the electronic properties of back-gated graphene field effect transistors (FETs) on Si/SiO(2) substrates. The excess charge on the graphene was observed by sweeping the gate voltage to determine the charge neutrality point in the graphene. Devices exposed to laboratory environment for several days were always found to be initially p-type. After approximately 20 h at 200 degrees C in approximately 5 x 10(-7) Torr vacuum, the FET slowly evolved to n-type behavior with a final excess electron density on the graphene of approximately 4 x 10(12) e/cm(2). This value is in excellent agreement with our theoretical calculations on SiO(2), where we have used molecular dynamics to build the SiO(2) structure and then density functional theory to compute the electronic structure. The essential theoretical result is that the SiO(2) has a significant surface state density just below the conduction band edge that donates electrons to the graphene to balance the chemical potential at the interface. An electrostatic model for the FET is also presented that produces an expression for the gate bias dependence of the carrier density.

We have studied the intrinsic doping level and gate hysteresis of graphene-based field effect transistors (FETs) fabricated over Si/SiO(2) substrates. It was found that the high p-doping level of graphene in some as-prepared devices can be reversed by vacuum degassing at room temperature or above depending on the degree of hydrophobicity and/or hydration of the underlying SiO(2) substrate. Charge neutrality point (CNP) hysteresis, consisting of the shift of the charge neutrality point (or Dirac peak) upon reversal of the gate voltage sweep direction, was also greatly reduced upon vacuum degassing. However, another type of hysteresis, consisting of the change in the transconductance upon reversal of the gate voltage sweep direction, persists even after long-term vacuum annealing at 200 °C, when SiO(2) surface-bound water is expected to be desorbed. We propose a mechanism for this transconductance hysteresis that involves water-related defects, formed during the hydration of the near-surface silanol groups in the bulk SiO(2), that can act as electron traps.

We report on experimental studies of NH3 adsorption/desorption on graphene surfaces. The study employs bottom-gated graphene field effect transistors supported on Si/SiO2 substrates. Detection of NH3 occurs through the shift of the source-drain resistance maximum ('Dirac peak') with the gate voltage. The observed shift of the Dirac peak toward negative gate voltages in response to NH3 exposure is consistent with a small charge transfer (f approximately 0.068 +/- 0.004 electrons per molecule at pristine sites) from NH3 to graphene. The desorption kinetics involves a very rapid loss of NH3 from the top surface and a much slower removal from the bottom surface at the interface with the SiO2 that we identify with a Fickian diffusion process.