Semiconducting transition metal dichalcogenides (TMDs) combine strong light-matter interaction with good chemical stability and scalable fabrication techniques, and are thus excellent prospects for optoelectronic, photonic and light-harvesting applications. Controllable fabrication of high-quality TMD monolayers with low defect content is still challenging and hinders their adoption for technological application. The optical properties of chemical vapor deposition (CVD) grown monolayer MoS$_2$ are largely influenced by the stoichiometry during CVD by controlled sulfurization of molybdenum (Mo) precursors. Here, we investigate how the sulfur concentration influences the sample morphology and, both globally and locally, their optical response. We confirm that samples grown under a Mo:S > 1:2 stoichiometric ratio have regular morphology facilitated by a moderate coverage of triangular monocrystals with excellent optical response. Our data-driven approach correlates growth conditions with crystal morphology and its optical response, providing a practical and necessary pathway to address the challenges towards the controlled synthesis of 2D TMDs and their alloys with desired optical and electronic properties.
Real-time monitoring is essential for understanding and eventually precise controlling of the growth of two dimensional transition-metal dichalcogenides (2D TMDCs). However, it is very challenging to carry out such kind of studies on chemical vapor deposition (CVD). Here, we report the first real time $in-situ$ study on the CVD growth of the 2D TMDCs. More specifically, CVD growth of molybdenum disulfide (MoS$_2$) monolayer on sapphire substrates has been monitored $in-situ$ using differential transmittance spectroscopy (DTS). The growth of the MoS$_2$ monolayer can be precisely followed by lo…
Atmospheric pressure chemical vapor deposition (APCVD) has been used extensively for synthesizing two-dimensional (2D) materials, due to its low cost and promise for high-quality monolayer crystal synthesis. However, the understanding of the reaction mechanism and the key parameters affecting the APCVD processes is still in its embryonic stage. Hence, the scalability of the APCVD method in achieving large scale continuous film remains very poor. Here, we use MoSe2 as a model system and present a fluid guided growth strategy for understanding and controlling the growth of 2D materials. Through …
We report, for CVD-grown monolayer MoS2, the very first results on temporal degradation of material and device performance under electrical stress. Both low and high field regimes of operation are explored at different temperatures, gate bias and stress cycles. During low field operation, current is found to saturate after hundreds of seconds of operation with the current decay time constant being a function of temperature and stress cycle. Current saturation after several seconds during low field operation occurs when a thermal equilibrium is established. However, high field operation, especi…
We characterize heat dissipation of supported molybdenum disulfide (MoS$_2$) monolayers grown by chemical vapor deposition by means of ambient-condition scanning thermal microscopy (SThM). We find that the thermal boundary conductance of the MoS$_2$ monolayers in contact with 300 nm of SiO$_2$ is around 4.6 $\pm$ 2 MW m$^{-2}$ K$^{-1}$. This value is in the low range of the values determined for exfoliated flakes with other techniques such as Raman thermometry, which span an order of magnitude (0.44-50 MW m$^{-2}$ K$^{-1}$), and underlines the dispersion of measurements. The sensitivity to the…
Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted great attention due to their physical and chemical properties that make them promising in electronics and optoelectronics. Because of the difficulties in controlling concentrations of solid precursors and spatially non-uniform growth dynamics, it is challenging to grow wafer-scale 2D TMDCs with good uniformity and reproducibility so far, which significantly hinders their practical use. Here we report a vertical chemical vapor deposition (VCVD) design to grow monolayer TMDCs with a uniform density and high quality over…
Graphene has been widely used in the form of micro-flakes to fabricate composite materials with enhanced mechanical properties. Due to the small size of the inclusions and their random orientation within the matrix, the superior mechanical properties of graphene cannot be fully exploited. Recently, attempts have been made to fabricate nanolaminate composites by interleaving large sheets of chemical vapor deposition (CVD) monolayer graphene between thin layers of polymer matrices. However, CVD graphene is inevitably accompanied by wrinkles that are formed in the synthesis process, and it remain…
Two-dimensional (2D) semiconductors have been proposed for heterogeneous integration with existing silicon technology; however, their chemical vapor deposition (CVD) growth temperatures are often too high. Here, we demonstrate direct CVD solid-source precursor synthesis of continuous monolayer (1L) MoS$_2$ films at 560 C in 50 min, within the 450-to-600 C, 2 h thermal budget window required for back-end-of-the-line compatibility with modern silicon technology. Transistor measurements reveal on-state current up to ~140 $\mathrm{μA/μm}$ at 1 V drain-to-source voltage for 100 nm channel lengths, …
Two-dimensional materials such as transitional metal dichalcogenides exhibit unique optical and electrical properties. Here we report on the varying optical properties of CVD grown MoS2 monolayer flakes with different shapes. In particular, it is observed that the perimeter and the central region of the flakes have non-uniform photoluminescence (PL) energy and intensity. We quantified these effects systematically and propose that thermally induced strain during growth is the origin. The strain relaxation after transfer of the MoS2 flakes supports this explanation. Detailed investigations of th…
The exploitation of the excellent intrinsic electronic properties of graphene for device applications is hampered by a large contact resistance between the metal and graphene. The formation of edge contacts rather than top contacts is one of the most promising solutions for realizing low ohmic contacts. In this paper the fabrication and characterization of edge contacts to large area CVD-grown monolayer graphene by means of optical lithography using CMOS compatible metals, i.e. Nickel and Aluminum is reported. Extraction of the contact resistance by Transfer Line Method (TLM) as well as the di…
We report on electronic transport in dual-gate, artificially stacked bilayer graphene field effect transistors (BiGFETs) fabricated from large-area chemical vapor deposited (CVD) graphene. The devices show enhanced tendency to current saturation, which leads to reduced minimum output conductance values. This results in improved intrinsic voltage gain of the devices when compared to monolayer graphene FETs. We employ a physics based compact model originally developed for Bernal stacked bilayer graphene FETs (BSBGFETs) to explore the observed phenomenon. The improvement in current saturation may…
Scalable fabrication of high quality photodetectors derived from synthetically grown monolayer transition metal dichalcogenides is highly desired and important for wide range of nanophotonics applications. We present here scalable fabrication of monolayer MoS2 photodetectors on sapphire substrates through an efficient process, which includes growing large scale monolayer MoS2 via chemical vapor deposition (CVD), and multi-step optical lithography for device patterning and high quality metal electrodes fabrication. In every measured device, we observed the following universal features: (i) negl…
Hexagonal boron nitride (h-BN) is a promising two-dimensional insulator with a large band gap and low density of charged impurities that is isostructural and isoelectronic with graphene. Here we report the chemical and atomic-scale structure of CVD-grown wafer-scale (~25 cm2) h-BN sheets ranging in thickness from 1-20 monolayers. Atomic-scale images of h-BN on Au and graphene/Au substrates obtained by scanning tunneling microscopy (STM) reveal high h-BN crystalline quality in monolayer samples. Further characterization of 1-20 monolayer samples indicates uniform thickness for wafer-scale areas…
Defects play a significant role in optical properties of semiconducting two-dimensional transition metal dichalcogenides (TMDCs). In ultra-thin MoSe2, a remarkable feature at ~250 cm-1 in Raman spectra is ascribed to be a defect-related mode. Recent attempts failed to explain the origin of this peak, leaving it being a mystery. Here in this work, we demonstrate that this peak is a Se vacancy induced defect mode. Heat effect and hydrogen etching are two main factors to introduce Se vacancies in CVD process of growing MoSe2. A phonon confinement model can well explain the behaviors of intrinsic …
We report for the first time the direct growth of Molybdenum disulfide (MoS$_2$) monolayers on nanostructured silicon-on-insulator waveguides. Our results indicate the possibility of utilizing the Chemical Vapour Deposition (CVD) on nanostructured photonic devices in a scalable process. Direct growth of 2D material on nanostructures rectifies many drawbacks of the transfer-based approaches. We show that the van der Waals materials grow conformally across the curves, edges, and the silicon-SiO$_2$ interface of the waveguide structure. Here, the waveguide structure used as a growth substrate is …
Recently, a contamination-free dry transfer method for graphene grown by chemical vapor deposition (CVD) has been reported that allows to directly pick-up graphene from the copper growth substrate using a flake of hexagonal boron nitride (hBN), resulting in ultrahigh charge carrier mobility and low overall doping. Here, we report that not only hBN, but also flakes of molybdenum disulfide (MoS$_2$) can be used to dry transfer graphene. This, on one hand, allows for the fabrication of complex van-der-Waals heterostructures using CVD graphene combined with different two-dimensional materials and,…
We performed Scanning Thermal Microscopy measurements on single layers of chemical-vapor-deposited -CVD- graphene supported by different substrates, namely SiO2, Al2O3 and PET using a double-scan technique to remove the contribution to the heat flux through the air and the cantilever. Then, by adopting a simple lumped-elements model, we developed a new method that allows determining, through a multi-step numerical analysis, the equivalent thermal properties of thermally conductive coatings of nanometric thickness. In this specific case we found that our CVD graphene is thermally equivalent, fo…
Unlike Si, 2-dimensional (2D) Transition Metal Dichalcogenides (TMDs) offer atomically thin channels for carrier transport in FETs. Despite advantages like superior gate control, steep sub-threshold swing and high carrier mobility offered by 2D FET channels, process related challenges like lack of selective doping techniques like implantation and CMOS compatible process for fabrication of 2D TMD based FETs hinder the anticipated viability of 2D semiconductor technology for future electronic applications. In this letter, we demonstrate a process oriented approach to realize superior ambipolarit…
We have studied the ambient air oxidation of chemical vapor deposition (CVD) grown monolayers of the semiconducting transition metal dichalcogenide (S-TMD) WS$_{2}$ using optical microscopy, laser scanning confocal microscopy (LSCM), photoluminescence (PL) spectroscopy, and atomic force microscopy (AFM). Monolayer WS$_{2}$ exposed to ambient conditions in the presence of light (typical laboratory ambient light for weeks, or typical PL spectroscopy map), exhibits damage due to oxidation which can be detected with the LSCM and AFM; though may not be evident in conventional optical microscopy due…