Graphene has emerged as an electronic material that is promising for device applications and for studying two-dimensional electron gases with relativistic dispersion near two Dirac points. Nonetheless, deviations from Dirac-like spectroscopy have been widely reported with varying interpretations. Here we show evidence for strain-induced spatial modulations in the local conductance of single-layer graphene on SiO(2) substrates from scanning tunneling microscopic (STM) studies. We find that strained graphene exhibits parabolic, U-shaped conductance vs bias voltage spectra rather than the V-shaped spectra expected for Dirac fermions, whereas V-shaped spectra are recovered in regions of relaxed graphene. Strain maps derived from the STM studies further reveal direct correlation with the local tunneling conductance. These results are attributed to a strain-induced frequency increase in the out-of-plane phonon mode that mediates the low-energy inelastic charge tunneling into graphene.
Current methods of chemical vapour deposition (CVD) of graphene on copper are complicated by multiple processing steps and by high temperatures required in both preparing the copper and inducing subsequent film growth. Here we demonstrate a plasma-enhanced CVD chemistry that enables the entire process to take place in a single step, at reduced temperatures (o420°C), and in a matter of minutes. Growth on copper foils is found to nucleate from arrays of well-aligned domains, and the ensuing films possess sub-nanometre smoothness, excellent crystalline quality, low strain, few defects and roomtemperature electrical mobility up to (6.0 ± 1.0) Â 10 4 cm 2 V À 1 s À 1 , better than that of large, single-crystalline graphene derived from thermal CVD growth. These results indicate that elevated temperatures and crystalline substrates are not necessary for synthesizing high-quality graphene.
Monolayer transition-metal dichalcogenides (TMDCs) in the 2H-phase are promising semiconductors for opto-valleytronic and opto-spintronic applications because of their strong spin-valley coupling. Here, we report detailed studies of opto-valleytronic properties of heterogeneous domains in CVD-grown monolayer WS2 single crystals. By illuminating WS2 with off-resonance circularly polarized light and measuring the resulting spatially resolved circularly polarized emission (P circ), we find significantly large circular polarization (P circ up to 60% and 45% for α- and β-domains, respectively) already at 300 K, which increases to nearly 90% in the α-domains at 80 K. Studies of spatially resolved photoluminescence (PL) spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, Kelvin-probe force microscopy, and conductive atomic force microscopy reveal direct correlation among the PL intensity, defect densities, and chemical potential, with the α-domains showing lower defect densities and a smaller work function by 0.13 eV than the β-domains. This work function difference indicates the occurrence of type-two band alignments between the α- and β-domains. We adapt a classical model to explain how electronically active defects may serve as nonradiative recombination centers and find good agreement between experiments and the model. Scanning tunneling microscopic/spectroscopic (STM/STS) studies provide further evidence for tungsten vacancies (WVs) being the primary defects responsible for the suppressed PL and circular polarization in WS2. These results therefore suggest a pathway to control the opto-valleytronic properties of TMDCs by means of defect engineering.
Hexagonal boron nitride (h-BN) is a promising two-dimensional insulator with a large band gap and low density of charged impurities that is isostructural and isoelectronic with graphene. Here we report the chemical and atomic-scale structure of CVD-grown wafer-scale (~25 cm 2 ) h-BN sheets
Plasma enhanced chemical vapor deposition (PECVD) techniques have been shown to be an efficient method to achieve single-step synthesis of high-quality monolayer graphene (MLG) without the need of active heating. Here we report PECVD-growth of single-crystalline hexagonal bilayer graphene (BLG) flakes and mm-size BLG films with the interlayer twist angle controlled by the growth parameters. The twist angle has been determined by three experimental approaches, including direct measurement of the relative orientation of crystalline edges between two stacked monolayers by scanning electron microscopy, analysis of the twist angle-dependent Raman spectral characteristics, and measurement of the Moiré period with scanning tunneling microscopy. In mm-sized twisted BLG (tBLG) films, the average twist angle can be controlled from 0 to approximately 20, and the angular spread for a given growth condition can be limited to < 7. Different work functions between MLG and BLG have been verified by the Kelvin probe force microscopy and ultraviolet photoelectron spectroscopy. Electrical measurements of back-gated field-effect-transistor devices based on small-angle tBLG samples revealed high-quality electric characteristics at 300 K and insulating temperature dependence down to 100 K. This controlled PECVD-growth of tBLG thus provides an efficient approach to investigate the effect of varying Moiré potentials on tBLG. 3
The realization of many promising technological applications of graphene and graphenebased nanostructures depends on the availability of reliable, scalable, high-yield and low-cost synthesis methods. Plasma enhanced chemical vapor deposition (PECVD) has been a versatile technique for synthesizing many carbon-based materials, because PECVD provides a rich chemical environment, including a mixture of radicals, molecules and ions from hydrocarbon precursors, which enables graphene growth on a variety of material surfaces at lower temperatures and faster growth than typical thermal chemical vapor deposition (T-CVD). Here we review recent advances in the PECVD techniques for synthesis of various graphene and graphene-based nanostructures, including horizontal growth of monolayer and multilayer graphene sheets, vertical growth of graphene nanostructures (VG-GNs) such as graphene nanostripes (GNSPs) with large aspect ratios, direct and selective deposition of monolayer and multi-layer graphene on nanostructured substrates, and growth of multi-wall carbon nanotubes (MWCNTs). By properly controlling the gas environment of the plasma, it is found that no active heating is necessary for the PECVD growth processes, and that highyield growth can take place in a single step on a variety of surfaces, including metallic, semiconducting and insulating materials. Phenomenological understanding of the growth mechanisms are described. Finally, challenges and promising outlook for further development in the PECVD techniques for graphene-based applications are discussed.
Long-term passivation of water-sensitive hybrid perovskites with monolayer graphene.
The environmental aging effect of doped graphene is investigated as a function of the organic doping species, humidity, and the number of graphene layers adjacent to the dopant by studies of the Raman spectroscopy, x-ray and ultraviolet photoelectron spectroscopy, scanning electron microscopy, infrared spectroscopy, and electrical transport measurements. It is found that higher humidity and structural defects induce faster degradation in doped graphene. Detailed analysis of the spectroscopic data suggest that the physical origin of the aging effect is associated with the continuing reaction of H 2 O molecules with the hygroscopic organic dopants, which leads to formation of excess chemical bonds, reduction in the doped graphene carrier density, and proliferation of damages from the graphene grain boundaries. These environmental aging effects are further shown to be significantly mitigated by added graphene layers.
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