Atmospheric-pressure chemical vapor deposition (CVD) is used to grow monolayer MoS 2 two-dimensional crystals at elevated temperatures on silicon substrates with a 300 nm oxide layer. Our CVD reaction is hydrogen free, with the sulfur precursor placed in a furnace separate from the MoO 3 precursor to individually control their heating profiles and provide greater flexibility in the growth recipe. We intentionally establish a sharp gradient of MoO 3 precursor concentration on the growth substrate to explore its sensitivity to the resultant MoS 2 domain growth within a relatively uniform temperature range. We find that the shape of MoS 2 domains is highly dependent upon the spatial location on the silicon substrate, with variation from triangular to hexagonal geometries. The shape change of domains is attributed to local changes in the Mo:S ratio of precursors (1:>2, 1:2, and 1:<2) and its influence on the kinetic growth dynamics of edges. These results improve our understanding of the factors that influence the growth of MoS 2 domains and their shape evolution.
Synthetic 2D crystal films grown by chemical vapor deposition are typically polycrystalline, and determining grain size within domains and continuous films is crucial for determining their structure. Here we show that grain boundaries in the 2D transition metal dichalcogenide WS2, grown by CVD, can be preferentially oxidized by controlled heating in air. Under our developed conditions, preferential degradation at the grain boundaries causes an increase in their physical size due to oxidation. This increase in size enables their clear and rapid identification using a standard optical microscope. We demonstrate that similar treatments in an Ar environment do no show this effect, confirming that oxidation is the main role in the structural change. Statistical analysis of grain boundary (GB) angles shows dominant mirror formation. Electrical biasing across the GB is shown to lead to changes at the GB and their observation under an optical microscope. Our approach enables high-throughput screening of as-synthesized WS2 domains and continuous films to determine their crystallinity and should enable improvements in future CVD growth of these materials.
Growing monolayer MoS2 films that are continuous with large domain sizes by chemical vapor deposition is one of the major challenges in 2D materials research at the moment. Here, we explore how atmospheric pressure CVD can be used to grow centimeter scale continuous films of monolayer MoS2 films directly on Si substrates with an oxide layer whilst also obtaining large domain sizes exceeding 20 μm within the films. This is achieved by orientating the growth substrate in a vertical position to improve the uniformity of precursor feed-stock compared to horizontally orientated growth substrates. This leads to continuous films of monolayer MoS2 over a significantly larger area without the need for low-pressure vacuum systems or volatile precursors. This provides important insights into novel approaches for maximizing domain sizes within MoS2 films, with concomitant large area uniform coverage.
Large amounts of waste heat generated in our fossil-fuel based economy can be converted into useful electric power by using thermoelectric generators. However, the low-efficiency, scarcity, high-cost and poor production scalability of conventional thermoelectric materials are hindering their mass deployment. Nanoengineering has proven to be an excellent approach for enhancing thermoelectric properties of abundant and cheap materials such as silicon. Nevertheless, the implementation of these nanostructures is still a major challenge especially for covering the large areas required for massive waste heat recovery. Here we present a family of nano-enabled materials in the form of large-area paper-like fabrics made of nanotubes as a cost-effective and scalable solution for thermoelectric generation. A case study of a fabric of p-type silicon nanotubes was developed showing a five-fold improvement of the thermoelectric figure of merit. Outstanding power densities above 100 W/m2 at 700 °C are therefore demonstrated opening a market for waste heat recovery.
We study how grain boundaries (GB) in chemical vapor deposition (CVD) grown monolayer WS2 influence the electroluminescence (EL) behavior in lateral source-drain devices under bias. Real time imaging of the WS2 EL shows arcing between the electrodes when probing across a GB, which then localizes at the GB region as it erodes under high bias conditions. In contrast, single crystal WS2 domains showed no signs of arcing or localized EL. Analysis of the eroded GB region shows the formation of micro- and nanoribbons across the monolayer WS2 domains. Comparison of the EL spectrum with the photoluminescence spectrum from the monolayer WS2 shows close agreement, indicating the EL emission comes from direct band gap excitonic recombination. These results provide important insights into EL devices that utilize CVD grown monolayer transition metal dichalcogenides when GBs are present in the active device region.
The combination of optimized and passivated Field Effect Transistors (FETs) based on carbon nanotubes (CNTs) together with the appropriate choice and immobilization strategy of aptamer receptors and buffer concentration have allowed the highly sensitive and real time biorecognition of proteins in a liquid-gated configuration. Specifically we have followed the biorecognition process of thrombin by its specific aptamer. The aptamer modified device is sensitive enough to capture a change in the electronic detection mechanism, one operating at low protein concentrations and the other in a higher target concentration range. The high sensitivity of the device is also sustained by the very low detection limits achieved (20 pM) and their high selectivity when other target proteins are used. Moreover, the experimental results have allowed us to quantify the equilibrium constant of the protein-aptamer binding and confirm its high affinity by using the Langmuir equation.
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