2D materials have been of considerable interest as new materials for device applications. Non‐volatile resistive switching applications of MoS2and WS2have been previously demonstrated; however, these applications are dramatically limited by high temperatures and extended times needed for the large‐area synthesis of 2D materials on crystalline substrates. The experimental results demonstrate a one‐step sulfurization method to synthesize MoS2and WS2at 550
Revealing the Brønsted-Evans-Polanyi relation in halide-activated fast MoS 2 growth toward millimeter-sized 2D crystals
Achieving large-size two-dimensional (2D) crystals is key to fully exploiting their remarkable functionalities and application potentials. Chemical vapor deposition growth of 2D semiconductors such as monolayer MoS 2 has been reported to be activated by halide salts, for which various investigations have been conducted to understand the underlying mechanism from different aspects. Here, we provide experimental evidence showing that the MoS 2 growth dynamics are halogen dependent through the Brønsted-Evans-Polanyi relation, based on which we build a growth model by considering MoS 2 edge passivation by halogens, and theoretically reproduce the trend of our experimental observations. These mechanistic understandings enable us to further optimize the fast growth of MoS 2 and reach record-large domain sizes that should facilitate practical applications.
more »
« less
- Award ID(s):
- 1807233
- NSF-PAR ID:
- 10382809
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 7
- Issue:
- 44
- ISSN:
- 2375-2548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract ° C in 15 min on sapphire wafers. Furthermore, a large area transfer of the synthesized thin films to SiO2/Si substrates is achieved. Following this, MoS2and WS2memristors are fabricated that exhibit stable non‐volatile switching and a satisfactory large on/off current ratio (103–105) with good uniformity. Tuning the sulfurization parameters (temperature and metal precursor thickness) is found to be a straightforward and effective strategy to improve the performance of the memristors. The demonstration of large‐scale MoS2and WS2memristors with a one‐step low‐temperature sulfurization method with simple strategy to tuning can lead to potential applications such as flexible memory and neuromorphic computing. -
Abstract The phase transitions of two-dimensional (2D) materials are key to the operation of many devices with applications including energy storage and low power electronics. Nanoscale confinement in the form of reduced thickness can modulate the phase transitions of 2D materials both in their thermodynamics and kinetics. Here, using in situ Raman spectroscopy we demonstrate that reducing the thickness of MoS 2 below five layers slows the kinetics of the phase transition from 2H- to 1T′-MoS 2 induced by the electrochemical intercalation of lithium. We observe that the growth rate of 1T′ domains is suppressed in thin MoS 2 supported by SiO 2 , and attribute this growth suppression to increased interfacial effects as the thickness is reduced below 5 nm. The suppressed kinetics can be reversed by placing MoS 2 on a 2D hexagonal boron nitride ( h BN) support, which readily facilitates the release of strain induced by the phase transition. Additionally, we show that the irreversible conversion of intercalated 1T′-MoS 2 into Li 2 S and Mo is also thickness-dependent and the stability of 1T′-MoS 2 is significantly increased below five layers, requiring a much higher applied electrochemical potential to break down 1T′-MoS 2 into Li 2 S and Mo nanoclusters.more » « less
-
more » « less
Abstract 2D materials‐based device performance is significantly affected by film non‐uniformity, especially for large area devices. Here, it investigates the dependence of large area 2D MoS2phototransistor performance on film morphology through correlative mapping. Monolayer MoS2films are quazi‐epitaxially synthesized on C‐plane sapphire (Al2O3) substrates by chemical vapor deposition, and the growth time and molybdenum trioxide MoO3precursor volume are varied to obtain variations in film morphology. Raman, photoluminescence, transmittance, and photocurrent maps are generated and compared with each other to obtain a holistic understanding of large area 2D optoelectronic device performance. For example, it shows that the photoluminescence peak shift and intensity can be used to investigate strain and other defects across multiple film morphologies, giving insight into their effects on the photogenerated current in these devices. It also combines photocurrent and absorption maps to generate large area high‐resolution external quantum efficiency and internal quantum efficiency maps for the devices. This study demonstrates the benefit of correlative mapping in the understanding and advancement of large area 2D material‐based electronic and optoelectronic devices.
-
null (Ed.)Two-dimensional (2D) molybdenum disulfide (MoS 2 ) layers are suitable for visible-to-near infrared photodetection owing to their tunable optical bandgaps. Also, their superior mechanical deformability enabled by an extremely small thickness and van der Waals (vdW) assembly allows them to be structured into unconventional physical forms, unattainable with any other materials. Herein, we demonstrate a new type of 2D MoS 2 layer-based rollable photodetector that can be mechanically reconfigured while maintaining excellent geometry-invariant photo-responsiveness. Large-area (>a few cm 2 ) 2D MoS 2 layers grown by chemical vapor deposition (CVD) were integrated on transparent and flexible substrates composed of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibers (TOCNs) by a direct solution casting method. These composite materials in three-dimensionally rollable forms exhibited a large set of intriguing photo-responsiveness, well preserving intrinsic opto-electrical characteristics of the integrated 2D MoS 2 layers; i.e. , light intensity-dependent photocurrents insensitive to illumination angles as well as highly tunable photocurrents varying with the rolling number of 2D MoS 2 layers, which were impossible to achieve with conventional photodetectors. This study provides a new design principle for converting 2D materials to three-dimensional (3D) objects of tailored functionalities and structures, significantly broadening their potential and versatility in futuristic devices.more » « less
-
Two-dimensional (2D) substrates decorated with metal nanoparticles offer new opportunities to achieve high-performance catalytic behavior. However, little is known on how the substrates control the nucleation and growth processes of the nanoparticles. This paper presents the visualization of dynamic nucleation and growth processes of gold nanoparticles on ultrathin MoS 2 nanoflakes by in situ liquid-cell transmission electron microscopy (TEM). The galvanic displacement resulting in Au nuclei formation on MoS 2 was observed in real time inside the liquid cell. We found that the growth mechanism of Au particles on pristine MoS 2 is in between diffusion-limited and reaction-limited, possibly due to the presence of electrochemical Ostwald ripening. A larger size distribution and more orientation variation is observed for the Au particles along the MoS 2 edge than on the interior. Differing from pristine MoS 2 , sulfur vacancies on MoS 2 induce Au particle diffusion and coalescence during the growth process. Density functional theory (DFT) calculations show that the size difference is because the exposed molybdenum atoms at the edge with dangling bonds can strongly interact with Au atoms, whereas sulfur atoms on the MoS 2 interior have no dangling bonds and weakly interact with gold atoms. In addition, S vacancies on MoS 2 generate strong nucleation centers that can promote diffusion and coalescence of Au nanoparticles. The present work provides key insights into the role of 2D materials in controlling the size and orientation of noble metal nanoparticles vital to the design of next generation catalysts.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1126/sciadv.abj3274
