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.
Solar nitrogen (N 2 ) fixation is the most attractive way for the sustainable production of ammonia (NH 3 ), but the development of a highly active, long-term stable and low-cost catalyst remains a great challenge. Current research efforts for N 2 reduction mainly focus on the metalbased catalysts using the electrochemical approach, while metalfree or solar-driven catalysts have been rarely explored. Herein, on the basis of a concept of electron "acceptance-donation", a metal-free photocatalyst, namely, boron (B) atom, decorated on the optically active graphitic-carbon nitride (B/g-C 3 N 4 ), for the reduction of N 2 is proposed by using extensive first-principles calculations. Our results reveal that gas phase N 2 can be efficiently reduced into NH 3 on B/g-C 3 N 4 through the enzymatic mechanism with a record low onset potential (0.20 V). Moreover, the B-decorated g-C 3 N 4 can significantly enhance the visible light absorption, rendering them ideal for solar-driven reduction of N 2 . Importantly, the as-designed catalyst is further demonstrated to hold great promise for synthesis due to its extremely high stability. Our work is the first report of metal-free single atom photocatalyst for N 2 reduction, offering cost-effective opportunities for advancing sustainable NH 3 production.
Molecular piezoelectrics are highly desirable for their easy and environment-friendly processing, light weight, low processing temperature, and mechanical flexibility. However, although 136 years have passed since the discovery in 1880 of the piezoelectric effect, molecular piezoelectrics with a piezoelectric coefficient comparable with piezoceramics such as barium titanate (BTO; ~190 picocoulombs per newton) have not been found. We show that trimethylchloromethyl ammonium trichloromanganese(II), an organic-inorganic perovskite ferroelectric crystal processed from aqueous solution, has a large of 185 picocoulombs per newton and a high phase-transition temperature of 406 kelvin (K) (16 K above that of BTO). This makes it a competitive candidate for medical, micromechanical, and biomechanical applications.
Molybdenum disulfide is considered as one of the most promising two-dimensional semiconductors for electronic and optoelectronic device applications. So far, the charge transport in monolayer molybdenum disulfide is dominated by extrinsic factors such as charged impurities, structural defects and traps, leading to much lower mobility than the intrinsic limit. Here we develop a facile low-temperature thiol chemistry route to repair the sulfur vacancies and improve the interface, resulting in significant reduction of the charged impurities and traps. High mobility 480 cm 2 V À 1 s À 1 is achieved in backgated monolayer molybdenum disulfide field-effect transistors at room temperature. Furthermore, we develop a theoretical model to quantitatively extract the key microscopic quantities that control the transistor performances, including the density of charged impurities, short-range defects and traps. Our combined experimental and theoretical study provides a clear path towards intrinsic charge transport in two-dimensional dichalcogenides for future high-performance device applications.
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