Xinran Wang

Hopping transport through defect-induced localized states in molybdenum disulphide

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.

Electrical characterization of back-gated bi-layer MoS2 field-effect transistors and the effect of ambient on their performances

Two-dimensional transition-metal dichalcogenides such as MoS2 are promising channel materials for transistor scaling. Here, we report the performance and environmental effects on back-gated bi-layer MoS2field-effect transistors. The devices exhibit Ohmic contacts with titanium at room temperature, on/off ratio higher than 107, and current saturation. Furthermore, we show that the devices are sensitive to oxygen and water in the ambient. Exposure to ambient dramatically reduces the on-state current by up to 2 orders of magnitude likely due to additional scattering centers from chemisorption on the defect sites of MoS2. We demonstrate that vacuum annealing can effectively remove the absorbates and reversibly recover the device performances. This method significantly reduces the large variations in MoS2 device caused by extrinsic factors.

Strong Photoluminescence Enhancement of MoS2 through Defect Engineering and Oxygen Bonding

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.

Towards intrinsic charge transport in monolayer molybdenum disulfide by defect and interface engineering

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 >80u2009cm(2)u2009V(-1)u2009s(-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.

Integrated digital inverters based on two-dimensional anisotropic ReS2 field-effect transistors

Semiconducting two-dimensional transition metal dichalcogenides are emerging as top candidates for post-silicon electronics. While most of them exhibit isotropic behaviour, lowering the lattice symmetry could induce anisotropic properties, which are both scientifically interesting and potentially useful. Here we present atomically thin rhenium disulfide (ReS2) flakes with unique distorted 1T structure, which exhibit in-plane anisotropic properties. We fabricated monolayer and few-layer ReS2 field-effect transistors, which exhibit competitive performance with large current on/off ratios (∼107) and low subthreshold swings (100u2009mV per decade). The observed anisotropic ratio along two principle axes reaches 3.1, which is the highest among all known two-dimensional semiconducting materials. Furthermore, we successfully demonstrated an integrated digital inverter with good performance by utilizing two ReS2 anisotropic field-effect transistors, suggesting the promising implementation of large-scale two-dimensional logic circuits. Our results underscore the unique properties of two-dimensional semiconducting materials with low crystal symmetry for future electronic applications.

Layer-by-Layer Thinning of MoS2 by Plasma

The electronic structures of two-dimensional materials are strongly dependent on their thicknesses; for example, there is an indirect to direct band gap transition from multilayer to single-layer MoS2. A simple, efficient, and nondestructive way to control the thickness of MoS2 is highly desirable for the study of thickness-dependent properties as well as for applications. Here, we present layer-by-layer thinning of MoS2 nanosheets down to monolayer by using Ar(+) plasma. Atomic force microscopy, high-resolution transmission electron microscopy, optical contrast, Raman, and photoluminescence spectra suggest that the top layer MoS2 is totally removed by plasma while the bottom layer remains almost unaffected. The evolution of Raman and photoluminescence spectra of MoS2 with thickness change is also investigated. Finally, we demonstrate that this method can be used to prepare two-dimensional heterostructures with periodical single-layer and bilayer MoS2. The plasma thinning of MoS2 is very reliable (with almost 100% success rate), can be easily scaled up, and is compatible with standard semiconductor process to generate heterostructures/patterns at nanometer scale, which may bring out interesting properties and new physics.

Two-dimensional quasi-freestanding molecular crystals for high-performance organic field-effect transistors

Two-dimensional atomic crystals are extensively studied in recent years due to their exciting physics and device applications. However, a molecular counterpart, with scalable processability and competitive device performance, is still challenging. Here, we demonstrate that high-quality few-layer dioctylbenzothienobenzothiophene molecular crystals can be grown on graphene or boron nitride substrate via van der Waals epitaxy, with precisely controlled thickness down to monolayer, large-area single crystal, low process temperature and patterning capability. The crystalline layers are atomically smooth and effectively decoupled from the substrate due to weak van der Waals interactions, affording a pristine interface for high-performance organic transistors. As a result, monolayer dioctylbenzothienobenzothiophene molecular crystal field-effect transistors on boron nitride show record-high carrier mobility up to 10u2009cm(2)u2009V(-1)u2009s(-1) and aggressively scaled saturation voltage ~1u2009V. Our work unveils an exciting new class of two-dimensional molecular materials for electronic and optoelectronic applications.

Top–down fabrication of sub-nanometre semiconducting nanoribbons derived from molybdenum disulfide sheets

Developments in semiconductor technology are propelling the dimensions of devices down to 10u2009nm, but facing great challenges in manufacture at the sub-10u2009nm scale. Nanotechnology can fabricate nanoribbons from two-dimensional atomic crystals, such as graphene, with widths below the 10u2009nm threshold, but their geometries and properties have been hard to control at this scale. Here we find that robust ultrafine molybdenum-sulfide ribbons with a uniform width of 0.35u2009nm can be widely formed between holes created in a MoS2 sheet under electron irradiation. In situ high-resolution transmission electron microscope characterization, combined with first-principles calculations, identifies the sub-1u2009nm ribbon as a Mo5S4 crystal derived from MoS2, through a spontaneous phase transition. Further first-principles investigations show that the Mo5S4 ribbon has a band gap of 0.77u2009eV, a Young’s modulus of 300GPa and can demonstrate 9% tensile strain before fracture. The results show a novel top–down route for controllable fabrication of functional building blocks for sub-nanometre electronics.

High‐Performance Monolayer WS2 Field‐Effect Transistors on High‐κ Dielectrics

The combination of high-quality Al2 O3 dielectric and thiol chemistry passivation can effectively reduce the density of interface traps and Coulomb impurities, leading to a significant improvement of the mobility and a transition of the charge transport from the insulating to the metallic regime. A record high mobility of 83 cm(2) V(-1) s(-1) (337 cm(2) V(-1) s(-1) ) is reached at room temperature (low temperature) for monolayer WS2 . A theoretical model for electron transport is also developed.

Planar carbon nanotube–graphene hybrid films for high-performance broadband photodetectors

Graphene has emerged as a promising material for photonic applications fuelled by its superior electronic and optical properties. However, the photoresponsivity is limited by the low absorption cross-section and ultrafast recombination rates of photoexcited carriers. Here we demonstrate a photoconductive gain of ∼105 electrons per photon in a carbon nanotube–graphene hybrid due to efficient photocarriers generation and transport within the nanostructure. A broadband photodetector (covering 400–1,550u2009nm) based on such hybrid films is fabricated with a high photoresponsivity of >100u2009Au2009W−1 and a fast response time of ∼100u2009μs. The combination of ultra-broad bandwidth, high responsivities and fast operating speeds affords new opportunities for facile and scalable fabrication of all-carbon optoelectronic devices.