We present a facile route which combines the functionalization of a highly oriented pyrolytic graphite surface with an atomic layer deposition (ALD) process to allow for conformal Al2O3 layers. While the trimethylaluminum (TMA)∕H2O process caused selective deposition only along step edges, the TMA∕O3 process began to provide nucleation sites on the basal planes of the surface. O3 pretreatment, immediately followed by the ALD process with TMA∕O3 chemistry, formed Al2O3 layers without any preferential deposition at the step edges. This is attributed to functionalization of graphene by ozone treatment, imparting a hydrophilic character which is desirable for ALD deposition.
We have investigated ozone adsorption on graphene using the ab initio density functional theory method. Ozone molecules adsorb on graphene basal plane with binding energy of 0.25 eV, and the physisorbed molecule can chemically react with graphene to form an epoxide group and an oxygen molecule. The activation energy barrier from physisorption to chemisorption is 0.72 eV, and the chemisorbed state has the binding energy of 0.33 eV. These binding energies and energy barrier indicate that the ozone adsorption on graphene is gentle and reversible. Atomic layer deposition experiment on ozone treated graphite has confirmed the presence of uniform hydrophilic groups on graphene basal plane. This finding can be applied to diverse chemical functionalization of graphene basal planes.
Integration of graphene field-effect transistors (GFETs) requires the ability to grow or deposit high-quality, ultrathin dielectric insulators on graphene to modulate the channel potential. Here, we study a novel and facile approach based on atomic layer deposition through ozone functionalization to deposit high-κ dielectrics (such as Al(2)O(3)) without breaking vacuum. The underlying mechanisms of functionalization have been studied theoretically using ab initio calculations and experimentally using in situ monitoring of transport properties. It is found that ozone molecules are physisorbed on the surface of graphene, which act as nucleation sites for dielectric deposition. The physisorbed ozone molecules eventually react with the metal precursor, trimethylaluminum to form Al(2)O(3). Additionally, we successfully demonstrate the performance of dual-gated GFETs with Al(2)O(3) of sub-5 nm physical thickness as a gate dielectric. Back-gated GFETs with mobilities of ~19,000 cm(2)/(V·s) are also achieved after Al(2)O(3) deposition. These results indicate that ozone functionalization is a promising pathway to achieve scaled gate dielectrics on graphene without leaving a residual nucleation layer.
The effect of H2O and O3 oxidants on the behavior of residual C and N-related impurities as well as Si out-diffusion and interfacial layer formation in atomic-layer-deposited La2O3 films grown at 250 °C were examined using in situ x-ray photoelectron spectroscopy. The silicate formation was suppressed in a La2O3 film grown using O3 compared to that deposited using H2O, but interfacial layer growth was enhanced. The accumulation of C and N-related residues with low binding energy, which originated from incomplete reactions, was suppressed in La2O3 films grown using O3. However, the use of O3 resulted in La-carbonate phase in film.
Articles you may be interested inCurrent, charge, and capacitance during scanning probe oxidation of silicon. I. Maximum charge density and lateral diffusionRecently, scanning resistive probe microscopy, which has a semiconducting resistor at the apex of the tip and observes surface charges directly, was newly proposed and fabricated. In order to optimize process parameters as well as to understand the mechanisms of the field induced resistance change in the resistive probe, the doping profile of resistive patterns is investigated by the use of Kelvin probe force microscopy. Overlapping space charge regions ͑O-SCRs͒ in between n + regions were observed. Decreased barrier heights in the structure of n + / O-SCR/ n + were also investigated. In particular, resistive patterns with diffusion times longer than 12 h were observed to have overlapped outdiffusion of As + ions, showing no formation of O-SCR in between n + regions. This was also confirmed by measurements of I-V characteristics.
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