Atomically thin molybdenum disulfide (MoS2), a member of the transition metal dichalcogenide (TMDC) family, has emerged as the prototypical two-dimensional (2D) semiconductor with a multitude of interesting properties and promising device applications spanning all realms of electronics and optoelectronics. While possessing inherent advantages over conventional bulk semiconducting materials (such as Si, Ge and III-Vs) in terms of enabling ultra-short channel and, thus, energy efficient field-effect transistors (FETs), the mechanically flexible and transparent nature of MoS2 makes it even more attractive for use in ubiquitous flexible and transparent electronic systems. However, before the fascinating properties of MoS2 can be effectively harnessed and put to good use in practical and commercial applications, several important technological roadblocks pertaining to its contact, doping and mobility (µ) engineering must be overcome. This paper reviews the important technologically relevant properties of semiconducting 2D TMDCs followed by a discussion of the performance projections of, and the major engineering challenges that confront, 2D MoS2-based devices. Finally, this review provides a comprehensive overview of the various engineering solutions employed, thus far, to address the all-important issues of contact resistance (RC), controllable and area-selective doping, and charge carrier mobility enhancement in these devices. Several key experimental and theoretical results are cited to supplement the discussions and provide further insight.

Electrostatic gating of two-dimensional (2D) materials with ionic liquids (ILs), leading to the accumulation of high surface charge carrier densities, has been often exploited in 2D devices. However, the intrinsic liquid nature of ILs, their sensitivity to humidity, and the stress induced in frozen liquids inhibit ILs from constituting an ideal platform for electrostatic gating. Here we report a lithium-ion solid electrolyte substrate, demonstrating its application in highperformance back-gated n-type MoS 2 and p-type WSe 2 transistors with sub-threshold values approaching the ideal limit of 60 mV/dec and complementary inverter amplifier gain of 34, the highest among comparable amplifiers. Remarkably, these outstanding values were obtained under 1 V power supply. Microscopic studies of the transistor channel using microwave impedance microscopy reveal a homogeneous channel formation, indicative of a smooth interface between the TMD and underlying electrolytic substrate. These results establish lithium-ion substrates as a promising alternative to ILs for advanced thin-film devices.

Molybdenum trioxide (MoO3), an important transition metal oxide (TMO), has been extensively investigated over the past few decades due to its potential in existing and emerging technologies, including catalysis, energy and data storage, electrochromic devices, and sensors. Recently, the growing interest in two-dimensional (2D) materials, often rich in interesting properties and functionalities compared to their bulk counterparts, has led to the investigation of 2D MoO3. However, the realization of large-area true 2D (single to few atom layers thick) MoO3 is yet to be achieved. Here, we demonstrate a facile route to obtain wafer-scale monolayer amorphous MoO3 using 2D MoS2 as a starting material, followed by UV–ozone oxidation at a substrate temperature as low as 120 °C. This simple yet effective process yields smooth, continuous, uniform, and stable monolayer oxide with wafer-scale homogeneity, as confirmed by several characterization techniques, including atomic force microscopy, numerous spectroscopy methods, and scanning transmission electron microscopy. Furthermore, using the subnanometer MoO3 as the active layer sandwiched between two metal electrodes, we demonstrate the thinnest oxide-based nonvolatile resistive switching memory with a low voltage operation and a high ON/OFF ratio. These results (potentially extendable to other TMOs) will enable further exploration of subnanometer stoichiometric MoO3, extending the frontiers of ultrathin flexible oxide materials and devices.

We investigate the role of growth temperature and metal/chalcogen flux in atmospheric pressure chemical vapor deposition growth of MoSe 2 and WSe 2 on Si/SiO 2 substrates. Using scanning electron microscopy and atomic force microscopy, we observe that the growth temperature and transition metal flux strongly influence the domain morphology, and the compact triangular or hexagonal domains ramify into branched structures as the growth temperature (metal flux) is decreased (increased). The competition between adatom attachment to the domain edges and diffusion of adatoms along the domain boundary determines the evolution of the observed growth morphology. Depending on the growth temperature and flux, two different branched structures fractals and dendritesgrow. The fractals (with a dimension of ∼1.67) obey a diffusion-limited aggregation mechanism, whereas the dendrites with a higher fractal dimension of ∼1.80 exhibit preferential growth along the symmetry-governed directions. The effect of chalcogen environment is studied, where a Se-rich condition helps restrict Mo-rich nucleus formation, promoting lateral growth. For a Se-deficient environment, several multilayer islands cluster on two-dimensional domains, suggesting a transition from lateral to vertical growth because of insufficient Se passivation. X-ray photoelectron spectroscopy analysis shows a near perfect stoichiometry (Mo/Se = 1:1.98) of MoSe 2 grown in a Se-rich environment, whereas in the Se-deficient condition, a ratio of Mo/Se = 1:1.68 is observed. This also supports the formation of metal-rich nuclei (Mo 1+x Se 2−x ) under Se-deficient conditions, leading to threedimensional clustering. Tuning the growth temperature and metal/chalcogen flux, we propose an optimized CVD growth window for synthesizing large-area Mo(W) selenide.

To achieve large area growth of transition metal dichalcogenides of uniform monolayer thickness, we demonstrate metal–organic chemical vapor deposition (MOCVD) growth under low pressure followed by a high-temperature sulfurization process under atmospheric pressure (AP). Following sulfurization, the MOCVD-grown continuous MoS 2 film transforms into compact triangular crystals of uniform monolayer thickness as confirmed from the sharp distinct photoluminescence peak at 1.8 eV. Raman and X-ray photoelectron spectroscopies confirm that the structural disorders and chalcogen vacancies inherent to the as-grown MOCVD film are substantially healed and carbon/oxygen contaminations are heavily suppressed. The as-grown MOCVD film has a Mo/S ratio of 1:1.6 and an average defect length of ∼1.56 nm, which improve to 1:1.97 and ∼21 nm, respectively, upon sulfurization. The effect of temperature and duration of the sulfurization process on the morphology and stoichiometry of the grown film is investigated in detail. Compared to the APCVD growth, this two-step growth process shows more homogenous distribution of the triangular monolayer MoS 2 domains across the entire substrate, while demonstrating comparable electrical performance.