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Register a new userMolecular Gas Adsorption Induced Carrier Transport Studies of Epitaxial Graphene using IR Reflection Spectroscopy
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We investigate molecular adsorption doping by electron withdrawing NO2 and electron donating NH3 on epitaxial graphene grown on C-face SiC substrates. Amperometric measurements show conductance changes upon introduction of molecular adsorbents on epitaxial graphene. Conductance changes are a trade-off between carrier concentration and scattering, and manifest at direct current and optical frequencies. We therefore investigate changes in the infrared (IR) reflection spectra to correlate these two frequency domains, as reflectance changes are due to a change of epitaxial graphene (EG) surface conductance. We match theory with experimental IR data and extract changes in carrier concentration and scattering due to gas adsorption. Finally, we separate the intraband and interband scattering contributions to the electronic transport under gas adsorption. The results indicate that, under gas adsorption, the influence of interband scattering cannot be neglected, even at DC.
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Variable-field Hall measurements were performed on epitaxial graphene grown on Si-face and C-face SiC. The carrier transport involves essentially a single-type of carrier in few-layer graphene, regardless of SiC face. However, in multi-layer graphene (MLG) grown on C-face SiC, the Hall measurements indicated the existence of several groups of carriers with distinct mobilities. Electrical transport in MLG can be properly described by invoking three independent conduction channels in parallel. Two of these are n- and p-type, while the third involves nearly intrinsic graphene. The carriers in this lightly doped channel have significantly higher mobilities than the other two.
The capability to control the type and amount of charge carriers in a material and, in the extreme case, the transition from metal to insulator is one of the key challenges of modern electronics. By employing angle resolved photoemission spectroscopy (ARPES) we find that a reversible metal to insulator transition and a fine tuning of the charge carriers from electrons to holes can be achieved in epitaxial bilayer and single layer graphene by molecular doping. The effects of electron screening and disorder are also discussed. These results demonstrate that epitaxial graphene is suitable for electronics applications, as well as provide new opportunities for studying the hole doping regime of the Dirac cone in graphene.
The electronic structure modifications of WSe2 upon NO2-adsorption at room and low temperatures were studied by means of photoelectron spectroscopy. We found only moderate changes in the electronic structure, which are manifested as an upward shift of the WSe2-related bands to the smaller binding energies. The observed effects are modelled within the density functional theory approach, where a weak adsorption energy of gas molecules on the surface of WSe2 was deduced. The obtained experimental data are explained as a valence bands polarisation effect, which causes their energy shift depending on the adsorption geometry and the formed dipole moment.
We show ~10x polariton-enhanced infrared reflectivity of epitaxial graphene on 4H-SiC, in SiCs restrahlen band (8-10um). By fitting measurements to theory, we extract the thickness, N, in monolayers (ML), momentum scattering time, Fermi level position of graphene and estimate carrier mobility. By showing that 1/root(ns), the carrier concentration/ML, we argue that scattering is dominated by short-range interactions at the SiC/graphene interface. Polariton formation finds application in near-field optical devices such as superlenses.
The adsorption energies and orientation of methanol on graphene are determined from first-principles density functional calculations. We employ the well-tested vdW-DF method that seamlessly includes dispersion interactions with all of the more close-ranged interactions that result in bonds like the covalent and hydrogen bonds. The adsorption of a single methanol molecule and small methanol clusters on graphene are studied at various coverages. Adsorption in clusters or at high coverages (less than a monolayer) is found to be preferable, with the methanol C-O axis approximately parallel to the plane of graphene. The adsorption energies calculated with vdW-DF are compared with previous DFT-D and MP2-based calculations for single methanol adsorption on flakes of graphene (polycyclic aromatic hydrocarbons). For the high coverage adsorption energies we also find reasonably good agreement with previous desorption measurements.
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