We developed a chemical route to produce graphene nanoribbons (GNR) with width below 10 nanometers, as well as single ribbons with varying widths along their lengths or containing lattice-defined graphene junctions for potential molecular electronics. The GNRs were solution-phase-derived, stably suspended in solvents with noncovalent polymer functionalization, and exhibited ultrasmooth edges with possibly well-defined zigzag or armchair-edge structures. Electrical transport experiments showed that, unlike single-walled carbon nanotubes, all of the sub-10-nanometer GNRs produced were semiconductors and afforded graphene field effect transistors with on-off ratios of about 10(7) at room temperature.
Graphene nanoribbons (GNRs) are materials with properties distinct from those of other carbon allotropes. The all-semiconducting nature of sub-10-nm GNRs could bypass the problem of the extreme chirality dependence of the metal or semiconductor nature of carbon nanotubes (CNTs) in future electronics. Currently, making GNRs using lithographic, chemical or sonochemical methods is challenging. It is difficult to obtain GNRs with smooth edges and controllable widths at high yields. Here we show an approach to making GNRs by unzipping multiwalled carbon nanotubes by plasma etching of nanotubes partly embedded in a polymer film. The GNRs have smooth edges and a narrow width distribution (10-20 nm). Raman spectroscopy and electrical transport measurements reveal the high quality of the GNRs. Unzipping CNTs with well-defined structures in an array will allow the production of GNRs with controlled widths, edge structures, placement and alignment in a scalable fashion for device integration.
Graphene is readily p-doped by adsorbates, but for device applications, it would be useful to access the n-doped material. Individual graphene nanoribbons were covalently functionalized by nitrogen species through high-power electrical joule heating in ammonia gas, leading to n-type electronic doping consistent with theory. The formation of the carbon-nitrogen bond should occur mostly at the edges of graphene where chemical reactivity is high. X-ray photoelectron spectroscopy and nanometer-scale secondary ion mass spectroscopy confirm the carbon-nitrogen species in graphene thermally annealed in ammonia. We fabricated an n-type graphene field-effect transistor that operates at room temperature.
Molybdenum disulphide is a novel two-dimensional semiconductor with potential applications in electronic and optoelectronic devices. However, the nature of charge transport in back-gated devices still remains elusive as they show much lower mobility than theoretical calculations and native n-type doping. Here we report a study of transport in few-layer molybdenum disulphide, together with transmission electron microscopy and density functional theory. We provide direct evidence that sulphur vacancies exist in molybdenum disulphide, introducing localized donor states inside the bandgap. Under low carrier densities, the transport exhibits nearest-neighbour hopping at high temperatures and variable-range hopping at low temperatures, which can be well explained under Mott formalism. We suggest that the low-carrier-density transport is dominated by hopping via these localized gap states. Our study reveals the important role of short-range surface defects in tailoring the properties and device applications of molybdenum disulphide.
We report on a strong photoluminescence (PL) enhancement of monolayer MoS2 through defect engineering and oxygen bonding. Micro-PL and Raman images clearly reveal that the PL enhancement occurs at cracks/defects formed during high-temperature annealing. The PL enhancement at crack/defect sites could be as high as thousands of times after considering the laser spot size. The main reasons of such huge PL enhancement include the following: (1) the oxygen chemical adsorption induced heavy p doping and the conversion from trion to exciton; (2) the suppression of nonradiative recombination of excitons at defect sites, which was verified by low-temperature PL measurements. First-principle calculations reveal a strong binding energy of ∼2.395 eV for an oxygen molecule adsorbed on a S vacancy of MoS2. The chemically adsorbed oxygen also provides a much more effective charge transfer (0.997 electrons per O2) compared to physically adsorbed oxygen on an ideal MoS2 surface. We also demonstrate that the defect engineering and oxygen bonding could be easily realized by mild oxygen plasma irradiation. X-ray photoelectron spectroscopy further confirms the formation of Mo-O bonding. Our results provide a new route for modulating the optical properties of two-dimensional semiconductors. The strong and stable PL from defects sites of MoS2 may have promising applications in optoelectronic devices.
Sub-10nm wide graphene nanoribbon field-effect transistors (GNRFETs) are studied systematically. All sub-10nm GNRs afforded semiconducting FETs without exception, with I on /I off ratio up to 10 6 and on-state current density as high as ~2000μA/μm. We estimated carrier mobility ~200cm 2 /Vs and scattering mean free path ~10nm in sub-10nm GNRs. Scattering mechanisms by edges, acoustic phonon and defects are discussed. The sub-10nm GNRFETs are comparable to small diameter (d≤~1.2nm) carbon nanotube FETs with Pd contacts in on-state current density and I on /I off ratio, but have the advantage of producing allsemiconducting devices.
The electrical and optical measurements, in combination with density functional theory calculations, show distinct layer-dependent semiconductor-to-semimetal evolution of 2D layered PtSe . The high room-temperature electron mobility and near-infrared photo-response, together with much better air-stability, make PtSe a versatile electronic 2D layered material.
Graphene is an intriguing material with properties that are distinct from those of other graphitic systems. The first samples of pristine graphene were obtained by 'peeling off' and epitaxial growth. Recently, the chemical reduction of graphite oxide was used to produce covalently functionalized single-layer graphene oxide. However, chemical approaches for the large-scale production of highly conducting graphene sheets remain elusive. Here, we report that the exfoliation-reintercalation-expansion of graphite can produce high-quality single-layer graphene sheets stably suspended in organic solvents. The graphene sheets exhibit high electrical conductance at room and cryogenic temperatures. Large amounts of graphene sheets in organic solvents are made into large transparent conducting films by Langmuir-Blodgett assembly in a layer-by-layer manner. The chemically derived, high-quality graphene sheets could lead to future scalable graphene devices.
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