Juhong Park

Growth of Large-Scale and Thickness-Modulated MoS2 Nanosheets

Two-dimensional MoS2 is a promising material for next-generation electronic and optoelectronic devices due to its unique electrical and optical properties including the band gap modulation with film thickness. Although MoS2 has shown excellent properties, wafer-scale production with layer control from single to few layers has yet to be demonstrated. The present study explored the large-scale and thickness-modulated growth of atomically thin MoS2 on Si/SiO2 substrates using a two-step sputtering-CVD method. Our process exhibited wafer-scale fabrication and successful thickness modulation of MoS2 layers from monolayer (0.72 nm) to multilayer (12.69 nm) with high uniformity. Electrical measurements on MoS2 field effect transistors (FETs) revealed a p-type semiconductor behavior with much higher field effect mobility and current on/off ratio as compared to previously reported CVD grown MoS2-FETs and amorphous silicon (a-Si) thin film transistors. Our results show that sputter-CVD is a viable method to synthesize large-area, high-quality, and layer-controlled MoS2 that can be adapted in conventional Si-based microfabrication technology and future flexible, high-temperature, and radiation hard electronics/optoelectronics.

Thickness modulated MoS2 grown by chemical vapor deposition for transparent and flexible electronic devices

Two-dimensional (2D) materials have been a great interest as high-performance transparent and flexible electronics due to their high crystallinity in atomic thickness and their potential for variety applications in electronics and optoelectronics. The present study explored the wafer scale production of MoS2 nanosheets with layer thickness modulation from single to multi-layer by using two-step method of metal deposition and CVD process. The formation of high-quality and layer thickness-modulated MoS2 film was confirmed by Raman spectroscopy, AFM, HRTEM, and photoluminescence analysis. The layer thickness was identified by employing a simple method of optical contrast value. The image contrast in green (G) channel shows the best fit as contrast increases with layer thickness, which can be utilized in identifying the layer thickness of MoS2. The presence of critical thickness of Mo for complete sulphurization, which is due to the diffusion limit of MoS2 transformation, changes the linearity of structural, ...

Centimeter Scale Patterned Growth of Vertically Stacked Few Layer Only 2D MoS2/WS2 van der Waals Heterostructure.

Two-dimensional (2D) van der Waal (vdW) heterostructures composed of vertically-stacked multiple transition metal dichalcogenides (TMDs) such as molybdenum disulfide (MoS2) and tungsten disulfide (WS2) are envisioned to present unprecedented materials properties unobtainable from any other material systems. Conventional fabrications of these hybrid materials have relied on the low-yield manual exfoliation and stacking of individual 2D TMD layers, which remain impractical for scaled-up applications. Attempts to chemically synthesize these materials have been recently pursued, which are presently limited to randomly and scarcely grown 2D layers with uncontrolled layer numbers on very small areas. Here, we report the chemical vapor deposition (CVD) growth of large-area (>2 cm2) patterned 2D vdW heterostructures composed of few layer, vertically-stacked MoS2 and WS2. Detailed structural characterizations by Raman spectroscopy and high-resolution/scanning transmission electron microscopy (HRTEM/STEM) directly evidence the structural integrity of two distinct 2D TMD layers with atomically sharp vdW heterointerfaces. Electrical transport measurements of these materials reveal diode-like behavior with clear current rectification, further confirming the formation of high-quality heterointerfaces. The intrinsic scalability and controllability of the CVD method presented in this study opens up a wide range of opportunities for emerging applications based on the unconventional functionalities of these uniquely structured materials.

2D MoS 2 as an efficient protective layer for lithium metal anodes in high-performance Li–S batteries

Among the candidates to replace Li-ion batteries, Li–S cells are an attractive option as their energy density is about five times higher (~2,600 Wh kg−1). The success of Li–S cells depends in large part on the utilization of metallic Li as anode material. Metallic lithium, however, is prone to grow parasitic dendrites and is highly reactive to several electrolytes; moreover, Li–S cells with metallic Li are also susceptible to polysulfides dissolution. Here, we show that ~10-nm-thick two-dimensional (2D) MoS2 can act as a protective layer for Li-metal anodes, greatly improving the performances of Li–S batteries. In particular, we observe stable Li electrodeposition and the suppression of dendrite nucleation sites. The deposition and dissolution process of a symmetric MoS2-coated Li-metal cell operates at a current density of 10 mA cm−2 with low voltage hysteresis and a threefold improvement in cycle life compared with using bare Li-metal. In a Li–S full-cell configuration, using the MoS2-coated Li as anode and a 3D carbon nanotube–sulfur cathode, we obtain a specific energy density of ~589 Wh kg−1 and a Coulombic efficiency of ~98% for over 1,200 cycles at 0.5 C. Our approach could lead to the realization of high energy density and safe Li-metal-based batteries.An ~10-nm-thick MoS2 layer stabilizes lithium metal anodes and the composite can be used in full-cell Li–S batteries with enhanced performances.

Synthesis of uniform single layer WS 2 for tunable photoluminescence

Two-dimensional transition metal dichalcogenides (2D TMDs) have gained great interest due to their unique tunable bandgap as a function of the number of layers. Especially, single-layer tungsten disulfides (WS2) is a direct band gap semiconductor with a gap of 2.1 eV featuring strong photoluminescence and large exciton binding energy. Although synthesis of MoS2 and their layer dependent properties have been studied rigorously, little attention has been paid to the formation of single-layer WS2 and its layer dependent properties. Here we report the scalable synthesis of uniform single-layer WS2 film by a two-step chemical vapor deposition (CVD) method followed by a laser thinning process. The PL intensity increases six-fold, while the PL peak shifts from 1.92 eV to 1.97 eV during the laser thinning from few-layers to single-layer. We find from the analysis of exciton complexes that both a neutral exciton and a trion increases with decreasing WS2 film thickness; however, the neutral exciton is predominant in single-layer WS2. The binding energies of trion and biexciton for single-layer WS2 are experimentally characterized at 35 meV and 60 meV, respectively. The tunable optical properties by precise control of WS2 layers could empower a great deal of flexibility in designing atomically thin optoelectronic devices.

Publisher Correction: 2D MoS 2 as an efficient protective layer for lithium metal anodes in high-performance Li–S batteries

In the version of this Article originally published, a technical error in typesetting led to the traces in Fig. 3a being trimmed and made to overlap. The figure has now been corrected with the traces as supplied by the authors; the original and corrected Fig. 3a are shown below. Also, in the last paragraph of the section “Mechanistic study on Li diffusion in MoS2” the authors incorrectly included the term ‘high-concentration’ in the text “the Li diffusion will be dominated by high-concentration Li migration on the surface of T-MoS2 with a much smaller energy barrier (0.155 eV) to overcome”. This term has now been removed from all versions of the Article. Finally, the authors have added an extra figure in the Supplementary Information (Supplementary Fig. 19) to show galvanostatic tests at 1 and 3 mA cm–2 for the MoS2-coated Li symmetric cells. The caption to Fig. 3 of the Article has been amended to reflect this, with the added wording “Galvanostatic tests at 1 and 3 mA cm–2 can be found in Supplementary Fig. 19.”

Composition-Tunable Synthesis of Large-Scale Mo1–xWxS2 Alloys with Enhanced Photoluminescence

Alloying two-dimensional transition metal dichalcogenides (2D TMDs) is a promising avenue for band gap engineering. In addition, developing a scalable synthesis process is essential for the practical application of these alloys with tunable band gaps in optoelectronic devices. Here, we report the synthesis of optically uniform and scalable single-layer Mo1- xW xS2 alloys by a two-step chemical vapor deposition (CVD) method followed by a laser thinning process. The amount of W content ( x) in the Mo1- xW xS2 alloy is systemically controlled by the co-sputtering technique. The post-laser process allows layer-by-layer thinning of the Mo1- xW xS2 alloys down to a single-layer; such a layer exhibits tunable properties with the optical band gap ranging from 1.871 to 1.971 eV with variation in the W content, x = 0 to 1. Moreover, the predominant exciton complexes, trions, are transitioned to neutral excitons with increasing W concentration; this is attributed to the decrease in excessive charge carriers with an increase in the W content of the alloy. Photoluminescence (PL) and Raman mapping analyses suggest that the laser-thinning of the Mo1- xW xS2 alloys is a self-limiting process caused by heat dissipation to the substrate, resulting in spatially uniform single-layer Mo1- xW xS2 alloy films. Our findings present a promising path for the fabrication of large-scale single-layer 2D TMD alloys and the design of versatile optoelectronic devices.