A chemical vapor deposition method is developed for thickness‐controlled (one to four layers), uniform, and continuous films of both defective gallium(II) sulfide (GaS): GaS0.87 and stoichiometric GaS. The unique degradation mechanism of GaS0.87 with X‐ray photoelectron spectroscopy and annular dark‐field scanning transmission electron microscopy is studied, and it is found that the poor stability and weak optical signal from GaS are strongly related to photo‐induced oxidation at defects. An enhanced stability of the stoichiometric GaS is demonstrated under laser and strong UV light, and by controlling defects in GaS, the photoresponse range can be changed from vis‐to‐UV to UV‐discriminating. The stoichiometric GaS is suitable for large‐scale, UV‐sensitive, high‐performance photodetector arrays for information encoding under large vis‐light noise, with short response time (<66 ms), excellent UV photoresponsivity (4.7 A W–1 for trilayer GaS), and 26‐times increase of signal‐to‐noise ratio compared with small‐bandgap 2D semiconductors. By comprehensive characterizations from atomic‐scale structures to large‐scale device performances in 2D semiconductors, the study provides insights into the role of defects, the importance of neglected material‐quality control, and how to enhance device performance, and both layer‐controlled defective GaS0.87 and stoichiometric GaS prove to be promising platforms for study of novel phenomena and new applications.
We show that reducing the degree of van der Waals overlapping in all 2D ultrathin lateral devices composed of graphene:WS2:graphene leads to significant increase in photodetector responsivity. This is achieved by directly growing WS2 using chemical vapor deposition (CVD) in prepatterned graphene gaps to create epitaxial interfaces. Direct-CVD-grown graphene:WS2:graphene lateral photodetecting transistors exhibit high photoresponsivities reaching 121 A/W under 2.7 × 105 mW/cm2 532 nm illumination, which is around 2 orders of magnitude higher than similar devices made by the layer-by-layer transfer method. The photoresponsivity of our direct-CVD-grown device shows negative correlation with illumination power under different gate voltages, which is different from similar devices made by the transfer method. We show that the high photoresponsivity is due to the lowering of effective Schottky barrier height by improving the contact between graphene and WS2. Furthermore, the direct CVD growth reduces overlapping sections of WS2:Gr and leads to more uniform lateral systems. This approach provides insights into scalable manufacturing of high-quality 2D lateral electronic and optoelectronic devices.
Cell sheet-mediated tissue regeneration is a promising approach for corneal reconstruction. However, the fragility of bioengineered corneal endothelial cell (CEC) monolayers allows us to take advantage of cross-linked porous gelatin hydrogels as cell sheet carriers for intraocular delivery. The aim of this study was to further investigate the effects of biopolymer concentrations (5–15 wt%) on the characteristic and safety of hydrogel discs fabricated by a simple stirring process combined with freeze-drying method. Results of scanning electron microscopy, porosity measurements, and ninhydrin assays showed that, with increasing solid content, the pore size, porosity, and cross-linking index of carbodiimide treated samples significantly decreased from 508±30 to 292±42 µm, 59.8±1.1 to 33.2±1.9%, and 56.2±1.6 to 34.3±1.8%, respectively. The variation in biopolymer concentrations and degrees of cross-linking greatly affects the Young’s modulus and swelling ratio of the gelatin carriers. Differential scanning calorimetry measurements and glucose permeation studies indicated that for the samples with a highest solid content, the highest pore wall thickness and the lowest fraction of mobile water may inhibit solute transport. When the biopolymer concentration is in the range of 5–10 wt%, the hydrogels have high freezable water content (0.89–0.93) and concentration of permeated glucose (591.3–615.5 µg/ml). These features are beneficial to the in vitro cultivation of CECs without limiting proliferation and changing expression of ion channel and pump genes such as ATP1A1, VDAC2, and AQP1. In vivo studies by analyzing the rabbit CEC morphology and count also demonstrate that the implanted gelatin discs with the highest solid content may cause unfavorable tissue-material interactions. It is concluded that the characteristics of cross-linked porous gelatin hydrogel carriers and their triggered biological responses are in relation to biopolymer concentration effects.
The solid progress in the study of a single two-dimensional (2D) material underpins the development for creating 2D material assemblies with various electronic and optoelectronic properties. We introduce an asymmetric structure by stacking monolayer semiconducting tungsten disulfide, metallic graphene, and insulating boron nitride to fabricate numerous red channel lightemitting devices (LEDs). All the 2D crystals were grown by chemical vapor deposition (CVD), which has great potential for future industrial scale-up. Our LEDs exhibit visibly observable electroluminescence (EL) at both 5.5 V forward and 7.0 V backward biasing, which correlates well with our asymmetric design. The red emission can last for at least several minutes, and the success rate of the working device that can emit detectable EL is up to 80%. In addition, we show that sample degradation is prone to happen when a continuing bias, much higher than the threshold voltage, is applied. Our success of using high-quality CVD-grown 2D materials for red light emitters is expected to provide the basis for flexible and transparent displays.
We show how an oxide passivating layer on the Cu surface before the growth of h-BN by chemical vapor deposition (CVD) can lead to increased domain sizes from 1 to 20 μm by reducing the nucleation density from 10 6 to 10 3 mm −2 . The h-BN domains within each Cu grain are welloriented, indicating an epitaxial relationship between the h-BN crystals and the Cu growth substrates that leads to larger crystal domains within the film of ∼100 μm. Continuous films are grown and show a high degree of monolayer uniformity. This CVD approach removes the need for low pressures, electrochemical polishing, and expensive substrates for large-area continuous films of h-BN monolayers, which is beneficial for industrial applications that require scalable synthesis.
Monolayer transition metal dichalcogenides (TMDs) have demonstrated great potential in next-generation electronics due to their unique optical and electronic properties. However, it remains challenging to produce uniform highquality TMDs over a large scale. The direct sulfurization method holds great promise in achieving large-scale synthesis, but the obtained materials suffer from small grain size and multilayer regions. Herein, low-cost glass substrate is used to achieve facile growth of large-area uniform and large-size monolayer MoS 2 crystals via a modified direct sulfurization method. We find that the ability of glass to incorporate predeposited precursors into its molten state is the key to the production of high-quality monolayer MoS 2 crystals. The monolayer MoS 2 crystals possess the largest average crystal size (∼100 μm) for MoS 2 grown by the direct sulfurization method, with large-area uniformity, which is only limited by the size of the substrate. A combination of low-cost, uniformity, scalability, simplicity, and high quality is achieved in our method which showed great promise for the development of wafer scale electronic devices based on 2D materials. Our work also provides a new look at the role substrates could play in the synthesis and the possibilities of using other glass or liquid substrates for the growth of high-quality 2D materials.
Tin disulfide crystals with layered two-dimensional (2D) sheets are grown by chemical vapor deposition using a novel precursor approach and integrated into all 2D transistors with graphene (Gr) electrodes. The Gr:SnS:Gr transistors exhibit excellent photodetector response with high detectivity and photoresponsivity. We show that the response of the all 2D photodetectors depends upon charge trapping at the interface and the Schottky barrier modulation. The thickness-dependent SnS measurements in devices reveal a transition from the interface-dominated response for thin crystals to bulklike response for the thicker SnS crystals, showing the sensitivity of devices fabricated using layered materials on the number of layers. These results show that SnS has photosensing performance when combined with Gr electrodes that is comparable to other 2D transition metal dichalcogenides of MoS and WS.
Doping of two-dimensional materials provides them tunable physical properties and widens their applications. Here, we demonstrate the postgrowth doping strategy in monolayer and bilayer tungsten disulfide (WS 2 ) crystals, which utilizes a metal exchange mechanism, whereby Sn atoms become substitutional dopants in the W sites by energetically favorable replacement. We achieve this using chemical vapor deposition techniques, where high-quality grown WS 2 single crystals are first grown and then subsequently reacted with a SnS precursor. Thermal control of the exchange doping mechanism is revealed, indicating that a sufficiently high enough temperature is required to create the S vacancies that are the initial binding sites for the SnS precursor and metal exchange occurrence. This results in a better control of dopant distribution compared to the tradition all-in-one approach, where dopants are added during the growth phase. The Sn dopants exhibit an n-type doping behavior in the WS 2 layers based on the decreased threshold voltage obtained from transistor device measurements. Annular dark-field scanning transmission electron microscopy shows that in bilayer WS 2 the Sn doping occurs only in the top layer, creating vertical heterostructures with atomic layer doping precision. This postgrowth modification opens up ways to selectively dope one layer at a time and construct mixed stoichiometry vertical heterojunctions in bilayer crystals.
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