Here we benchmark device-to-device variation in field-effect transistors (FETs) based on monolayer MoS2 and WS2 films grown using metal-organic chemical vapor deposition process. Our study involves 230 MoS2 FETs and 160 WS2 FETs with channel lengths ranging from 5 μm down to 100 nm. We use statistical measures to evaluate key FET performance indicators for benchmarking these two-dimensional (2D) transition metal dichalcogenide (TMD) monolayers against existing literature as well as ultra-thin body Si FETs. Our results show consistent performance of 2D FETs across 1 × 1 cm2 chips owing to high quality and uniform growth of these TMDs followed by clean transfer onto device substrates. We are able to demonstrate record high carrier mobility of 33 cm2 V−1 s−1 in WS2 FETs, which is a 1.5X improvement compared to the best reported in the literature. Our experimental demonstrations confirm the technological viability of 2D FETs in future integrated circuits.
Atomically thin transition metal dichalcogenides (TMDs) are of interest for next-generation electronics and optoelectronics. Here, we demonstrate device-ready synthetic tungsten diselenide (WSe) via metal-organic chemical vapor deposition and provide key insights into the phenomena that control the properties of large-area, epitaxial TMDs. When epitaxy is achieved, the sapphire surface reconstructs, leading to strong 2D/3D (i.e., TMD/substrate) interactions that impact carrier transport. Furthermore, we demonstrate that substrate step edges are a major source of carrier doping and scattering. Even with 2D/3D coupling, transistors utilizing transfer-free epitaxial WSe/sapphire exhibit ambipolar behavior with excellent on/off ratios (∼10), high current density (1-10 μA·μm), and good field-effect transistor mobility (∼30 cm·V·s) at room temperature. This work establishes that realization of electronic-grade epitaxial TMDs must consider the impact of the TMD precursors, substrate, and the 2D/3D interface as leading factors in electronic performance.
A multistep diffusion-mediated process was developed to control the nucleation density, size, and lateral growth rate of WSe domains on c-plane sapphire for the epitaxial growth of large area monolayer films by gas source chemical vapor deposition (CVD). The process consists of an initial nucleation step followed by an annealing period in HSe to promote surface diffusion of tungsten-containing species to form oriented WSe islands with uniform size and controlled density. The growth conditions were then adjusted to suppress further nucleation and laterally grow the WSe islands to form a fully coalesced monolayer film in less than 1 h. Postgrowth structural characterization demonstrates that the WSe monolayers are single crystal and epitaxially oriented with respect to the sapphire and contain antiphase grain boundaries due to coalescence of 0° and 60° oriented WSe domains. The process also provides fundamental insights into the two-dimensional (2D) growth mechanism. For example, the evolution of domain size and cluster density with annealing time follows a 2D ripening process, enabling an estimate of the tungsten-species surface diffusivity. The lateral growth rate of domains was found to be relatively independent of substrate temperature over the range of 700-900 °C suggesting a mass transport limited process, however, the domain shape (triangular versus truncated triangular) varied with temperature over this same range due to local variations in the Se/W adatom ratio. The results provide an important step toward atomic level control of the epitaxial growth of WSe monolayers in a scalable process that is suitable for large area device fabrication.
Realization of wafer-scale single-crystal films of transition metal dichalcogenides (TMDs) such as WS 2 requires epitaxial growth and coalescence of oriented domains to form a continuous monolayer. The domains must be oriented in the same crystallographic direction on the substrate to inhibit the formation of inversion domain boundaries (IDBs), which are a common feature of layered chalcogenides. Here we demonstrate fully coalesced unidirectional WS 2 monolayers on 2 in. diameter c-plane sapphire by metalorganic chemical vapor deposition using a multistep growth process to achieve epitaxial WS 2 monolayers with low in-plane rotational twist (0.09°). Transmission electron microscopy analysis reveals that the WS 2 monolayers are largely free of IDBs but instead have translational boundaries that arise when WS 2 domains with slightly offset lattices merge together. By regulating the monolayer growth rate, the density of translational boundaries and bilayer coverage were significantly reduced. The unidirectional orientation of domains is attributed to the presence of steps on the sapphire surface coupled with growth conditions that promote surface diffusion, lateral domain growth, and coalescence while preserving the aligned domain structure. The transferred WS 2 monolayers show neutral and charged exciton emission at 80 K with negligible defect-related luminescence. Back-gated WS 2 field effect transistors exhibited an I ON / OFF of ∼10 7 and mobility of 16 cm 2 /(V s). The results demonstrate the potential of achieving wafer-scale TMD monolayers free of inversion domains with properties approaching those of exfoliated flakes.
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