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Dynamic vision perception and processing (DVPP) is in high demand by booming edge artificial intelligence. However, existing imaging systems suffer from low efficiency or low compatibility with advanced machine vision techniques. Here, we propose a reconfigurable bipolar image sensor (RBIS) for in-sensor DVPP based on a two-dimensional WSe2/GeSe heterostructure device. Owing to the gate-tunable and reversible built-in electric field, its photoresponse shows bipolarity as being positive or negative. High-efficiency DVPP incorporating front-end RBIS and back-end CNN is then demonstrated. It shows a high recognition accuracy of over 94.9% on the derived DVS128 data set and requires much fewer neural network parameters than that without RBIS. Moreover, we demonstrate an optimized device with a vertically stacked structure and a stable nonvolatile bipolarity, which enables more efficient DVPP hardware. Our work demonstrates the potential of fabricating DVPP devices with a simple structure, high efficiency, and outputs compatible with advanced algorithms.
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Visible-blind ultraviolet (UV) light detection has a wide application range in scenes like space environment monitoring and medical imaging. To realize miniaturized UV detectors with high performance and high integration ability, new device structures without bulky light filters need to be developed based on advanced mechanisms. Here the unipolar barrier van der Waals heterostructure (UB-vdWH) photodetector is reported that realizes filter-free visible-blind UV detection with good stability, robustness, selectivity, and high detection performance. The UB-vdWH shows a responsivity of 2452 A W-1, a photo on-off ratio of 2.94 × 105 and a detectivity of 1.26 × 1015 Jones as a UV detector, owing to the intentionally designed barrier height that suppresses dark current and photoresponse to visible light during the transport process. The good performance remains intact during 104 test cycles or even under high temperatures, which proves the stability, and robustness of the UB-vdWH, thus shows the huge potential for a wider application range.
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In-sensor computing hardware based on emerging reconfigurable photosensors can effectively reduce redundant data and decrease power consumption, which can greatly promote the evolution of machine vision. However, because of the complex device structures and low integration abilities, the common architectures mainly lie in two dimensions, resulting in low time and area efficiencies. Here we propose a three-dimensional (3D) neuromorphic photosensor array for parallel in-sensor image processing. It is constructed on a vertical Graphite/CuInP2S6/Graphite photosensor unit, where the directional Cu+ ion migrations after voltage pulse programming enable a reconfigurable photovoltaic effect and an in-sensor computing capability. With a memristor-like device structure, van der Waals interfaces, and a high uniformity with a low crosstalk problem, a 10 × 10 array is fabricated for intelligent image recognition. Furthermore, using a vertically stacked 3D 3 × 3 × 3 array, we demonstrate an in-sensor convolution strategy with high time and area efficiencies.
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Iron oxyhydroxide has been considered an auspicious electrocatalyst for the oxygen evolution reaction (OER) in alkaline water electrolysis due to its suitable electronic structure and abundant reserves. However, Fe-based materials seriously suffer from the tradeoff between activity and stability at a high current density above 100 mA cm-2 . In this work, the Ce atom is introduced into the amorphous iron oxyhydroxide (i.e., CeFeOx Hy ) nanosheet to simultaneously improve the intrinsic electrocatalytic activity and stability for OER through regulating the redox property of iron oxyhydroxide. In particular, the Ce substitution leads to the distorted octahedral crystal structure of CeFeOx Hy , along with a regulated coordination site. The CeFeOx Hy electrode exhibits a low overpotential of 250 mV at 100 mA cm-2 with a small Tafel slope of 35.1 mVdec-1 . Moreover, the CeFeOx Hy electrode can continuously work for 300 h at 100 mA cm-2 . When applying the CeFeOx Hy nanosheet electrode as the anode and coupling it with the platinum mesh cathode, the cell voltage for overall water splitting can be lowered to 1.47 V at 10 mA cm-2 . This work offers a design strategy for highly active, low-cost, and durable material through interfacing high valent metals with earth-abundant oxides/hydroxides.
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Tin telluride (SnTe), as a narrow bandgap semiconductor material, has great potential for developing photodetectors with wide spectra and ultra-fast response. At the same time, it is also an important topological crystal insulator material, with different topological surface states on several common surfaces. Here, we introduce different Sn sources and control the growth of regular SnTe nanosheets along the (100) and (111) planes through the atmospheric pressure chemical vapor deposition method. It has been proven through various characterizations that the synthesized SnTe is a high-quality single crystal. In addition, the angular resolved Raman spectra of SnTe nanosheets grown on different crystal planes are first demonstrated. The experimental results showed that square SnTe nanosheets grown along the (100) plane exhibit in-plane anisotropy. At the same time, we use micro-nanofabrication technology to manufacture SnTe-based field effect transistors and photodetectors to explore their electrical and optoelectronic properties. It has been confirmed that transistors based on grown SnTe nanosheets exhibit p-type semiconductor characteristics and have a high response to infrared light. This work provides a new approach for the controllable synthesis of SnTe and adds new content to the research of SnTe-based infrared detectors.
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Two-dimensional semiconductors have great potential for beyond-silicon electronics. However, because of the lack of controllable doping methods, Fermi level pinning, and van der Waals (vdW) gaps at the metal-semiconductor interfaces, these devices exhibit high electrical contact resistances, restricting their practical applications. Here, we report a general contact-resistance-lowering strategy by constructing vertical metal-semiconductor-metal memristor structures at the contact regions and setting them into a nonvolatile low-resistance state through a memristive forming process. Through this, we reduce the contact resistances of MoS2 field-effect transistors (FETs) by at least one order of magnitude and improve the on-state current densities of MoTe2 FETs by about two orders of magnitude. We also demonstrate that this strategy is applicable to other two-dimensional semiconductors, including MoSe2, WS2, and WSe2, and a variety of contact metals, including Au, Cu, Ni, and Pd. The good stability and universality indicate the great potential for technological applications.
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Photodetectors based on low-dimensional materials usually suffer from serious optical power-dependent photoresponse and low reliability, particularly in the ultraviolet regime. The barrier photodetector is an effective and reliable strategy where the barrier layer can block the low-energy charge carriers while allowing for a flow of the high-energy photocarriers. Here, vertical barrier heterostructure photodetectors (VBHPs), consisting of a graphene bottom electrode, a MoS2 light absorber, and an h-BN energy barrier, for reliable, robust, and high-performance ultraviolet detection are reported. The asymmetric barrier distribution in the conduction/valence band at the MoS2 /h-BN interface results in an ultralow noise current of 1.69 × 10-15 A Hz-1/2 at room temperature, stable photo on/off states exceeding 104 cycles at 300 K and 400 K, a light power-independent high responsivity of 416.2 mA W-1 at 360 nm, a high photo on-off ratio of 1.2 × 105 at 360 nm, high measured detectivities (3.2 × 1010 Jones at 266 nm and 9.9 × 1010 Jones at 360 nm), and wide linear dynamic ranges. The VBHPs show a high potential for new-type reliable ultraviolet detection.
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As an important metal phosphides material, 2D tin phosphides (SnPx 0 < x ≤ 3) have been theoretically predicted to have intriguing physicochemical properties and potential applications in electronics, optoelectronics, and energy fields. However, the synthesis of high-quality 2D SnP single crystal has not been reported due to the lack of efficiency and reliable growth method. Here, a facile atmospheric pressure chemical vapor deposition (APCVD) method is developed to realize the growth of high-quality 2D SnP nanosheets, by employing tin (Sn) foil as both liquid metal substrates and reaction precursor. Temperature-dependent and angle-resolved polarization Raman spectra observed Raman peaks located at 142.6, 303.3, and 444.2 cm-1 are concluded to belong to A1g mode, which are consistent with the theoretical calculation results. Moreover, the field-effect transistor (FET) devices based on SnP nanosheets show a typical n-type characteristic with an on/off ratio of 103 at 200 K. SnP nanosheets also demonstrate excellent photoresponse performance under the illumination of 473, 532, and 639 nm lasers, which can be tuned by Vgs , Vds , and light power density. It is believed that these findings can provide the first-hand experimental information for the future study of 2D SnP nanosheets.
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Intrinsic two-dimensional (2D) magnetic materials own strong long-range magnetism while their characteristics of the ultrathin thickness and smooth surface provide an ideal platform for manipulating the magnetic properties at 2D limit. This makes them to be potential candidates in various spintronic applications compared to their corresponding bulk counterparts. The discovery of magnetic ordering in 2D CrI3and Gr2Ge2Te6nanostructures stimulated tremendous research interest in both experimental and theoretical studies on various intrinsic magnets at 2D limit. This review gives a comprehensive overview of the recent progress on the emergent 2D magnets and heterostructures. Firstly, several kinds of typical 2D magnetic materials discovered in the last few years and their fabrication methods are summarized in detail. Secondly, the current strategies for manipulating magnetic properties in 2D materials are further discussed. Then, the recent advances on the construction of representative van der Waals magnetic heterostructures and their respective performance are provided. With the hope of motivating the researchers in this area, we finally offered the challenges and outlook on 2D magnetism.
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Two-dimensional materials have been widely used in electronics due to their electrical properties that are not accessible in traditional materials. Here, we present the first demonstration of logic functions of unipolar memristors made of functionalized HfSe2-xOx flakes and memtransistors made of MoS2/graphene/HfSe2-xOx van der Waals heterostructures. The two-terminal memristors exhibit stable unipolar switching behavior with high switching ratio (>106), high operating temperature (106 °C), long-term endurance (>104 s), and multibit data storage and can operate as memory latches and logic gates. Benefiting from these superior memristive properties, the three-terminal heterostructure memtransistors show wide tunability in electrical switching behaviors, which can simultaneously implement logic operation and data storage. Finally, we investigate their application prospect in logical units with memory capability, such as D-type flip-flop. These results demonstrate the potential of two-dimensional materials for resistive switching applications and open up an avenue for future in-memory computing.
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Nanomaterials have gained plenty of research interest because of their excellent performance, which is derived from their small size and special structure. In practical applications, to acquire nanomaterials with high performance, many methods have been used to modulate the structure and components of materials. To date, ion beam techniques have extensively been applied for modulating the performance of various nanomaterials. Energetic ion beams can modulate the surface morphology and chemical components of nanomaterials. In addition, ion beam techniques have also been used to fabricate nanomaterials, including 2D materials, nanoparticles, and nanowires. Compared with conventional methods, ion beam techniques, including ion implantation, ion irradiation, and focused ion beam, are all pure physical processes; these processes do not introduce any impurities into the target materials. In addition, ion beam techniques exhibit high controllability and repeatability. Here, recent progress in ion beam techniques for nanomaterial surface modification is systematically summarized and existing challenges and potential solutions are presented.
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Two-dimensional layered materials (2DLMs) have attracted a tremendous amount of attention as photodetectors due to their fascinating features, including high potentials in new-generation electronic devices, wide coverage of bandgaps, ability to construct van der Waals heterostructures, extraordinary light-mass interaction, strong mechanical flexibility, and the capability of enabling synthesis of 2D nonlayered materials. Until now, most attention has been focused on the well-known graphene and transition metal dichalcogenides (TMDs). However, a growing number of functional materials (more than 5619) with novel optoelectronic and electronic properties are being re-discovered, thereby widening the horizon of 2D libraries. In addition to showing common features of 2DLMs, these new 2D members may bring new opportunities to their well-known analogues, like wider bandgap coverage, direct bandgaps independence with thickness, higher mechanical flexibility, and new photoresponse phenomena. The impressive results communicated so far testify that they have shown high potentials with photodetections covering THz, IR, visible, and UV ranges with comparable or even higher performances than well-known TMDs. Here, we give a comprehensive review on the state-of-the-art photodetections of two-dimensional materials beyond graphene and TMDs. The review is organized as follows: fundamentals of photoresponse first are discussed, followed by detailed photodetections of new 2D members including both layered and non-layered ones. After that, photodiodes and hybrid structures based on these new 2D materials are summarized. Then, the integration of these 2D materials with flexible substrates is reviewed. Finally, we conclude with the current research status of this area and offer our perspectives on future developments. We hope that, through reading this manuscript, readers will quickly have a comprehensive view on this research area.
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The rational design of Earth abundant electrocatalysts for efficiently catalyzing hydrogen evolution reaction (HER) is believed to lead to the generation of carbon neutral energy carrier. Owing to their fascinating chemical and physical properties, transition metal dichalcogenides (TMDs) are widely studied for this purpose. Of particular note is that doping by foreign atom can bring the advent of electronic perturbation, which affects the intrinsic catalytic property. Hence, through doping, the catalytic activity of such materials could be boosted. A rational synthesis approach that enables phosphorous atom to be doped into WS2 without inducing phase impurity to form WS2(1-x) P2x nanoribbon (NRs) is herein reported. It is found that the WS2(1-x) P2x NRs exhibit considerably enhanced HER performance, requiring only -98 mV versus reversible hydrogen electrode to achieve a current density of -10 mA cm-2 . Such a high performance can be attributed to the ease of H-atom adsorption and desorption due to intrinsically tuned WS2 , and partial formation of NRs, a morphology wherein the exposure of active edges is more pronounced. This finding can provide a fertile ground for subsequent works aiming at tuning intrinsic catalytic activity of TMDs.
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2D layered semiconducting materials (2DLSMs) represent the thinnest semiconductors, holding many novel properties, such as the absence of surface dangling bonds, sizable band gaps, high flexibility, and ability of artificial assembly. With the prospect of bringing revolutionary opportunities for electronic and optoelectronic applications, 2DLSMs have prospered over the past twelve years. From materials preparation and property exploration to device applications, 2DLSMs have been extensively investigated and have achieved great progress. However, there are still great challenges for high-performance devices. In this review, we provide a brief overview on the recent breakthroughs in device optimization based on 2DLSMs, particularly focussing on three aspects: device configurations, basic properties of channel materials, and heterostructures. The effects from device configurations, i.e., electrical contacts, dielectric layers, channel length, and substrates, are discussed. After that, the affect of the basic properties of 2DLSMs on device performance is summarized, including crystal defects, crystal symmetry, doping, and thickness. Finally, we focus on heterostructures based on 2DLSMs. Through this review, we try to provide a guide to improve electronic and optoelectronic devices of 2DLSMs for achieving practical device applications in the future.
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Molybdenum disulfide (MoS2) has attracted a great deal of attention in optoelectronic applications due to its high mobility, low off-state current and high on/off ratio. However, its intrinsic large bandgap limits its application in infrared detection. Here, we have developed a high-performance infrared photodetector by integrating nonlayered PbS and layered MoS2 nanostructures via van der Waals epitaxy. Density functional theory (DFT) calculations indicate that PbS nanoplates are in contact with MoS2 edges through strong chemical hybridization, which is expected to offer a fast transmission path for carriers that enhances the response speed. The phototransistor exhibits a fast response (τrising = τdecay = 7.8 ms) as well as high photoresponsivity (4.5 × 104 A·W-1) and Ilight/Idark (1.3 × 102) in the near-infrared spectral region at room temperature. In particular, the detectivity (D*) is as high as 3 × 1013 Jones, which is even better than that of commercial Si and InGaAs photodetectors. Furthermore, by controlling the growth and microfabrication patterning, periodic device arrays of PbS-MoS2 that are capable of infrared detection are achieved on Si/SiO2 substrates. Our work provides a possible method for the integration of photodetector arrays on Si-based electronic devices and lays a solid foundation for the practical applications of MoS2-based devices in the future.
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Transition metal dichalcogenides (TMDs), as one of potential electrocatalysts for hydrogen evolution reaction (HER), have been extensively studied. Such TMD-based ternary materials are believed to engender optimization of hydrogen adsorption free energy to thermoneutral value. Theoretically, cobalt is predicted to actively promote the catalytic activity of WS2 . However, experimentally it requires systematic approach to form Cox W(1- x ) S2 without any concomitant side phases that are detrimental for the intended purpose. This study reports a rational method to synthesize pure ternary Cox W(1- x ) S2 nanosheets for efficiently catalyzing HER. Benefiting from the modification in the electronic structure, the resultant material requires overpotential of 121 mV versus reversible hydrogen electrode (RHE) to achieve current density of 10 mA cm(-2) and shows Tafel slope of 67 mV dec(-1) . Furthermore, negligible loss of activity is observed over continues electrolysis of up to 2 h demonstrating its fair stability. The finding provides noticeable experimental support for other computational reports and paves the way for further works in the area of HER catalysis based on ternary materials.
Assuntos
Eletroquímica/métodos , Hidrogênio/química , Nanoestruturas/química , Eletrodos , Elementos de Transição/químicaRESUMO
Pb(1-x)Sn(x)Te is a unique topological crystalline insulator (TCI) that undergoes a topological phase transition from topological trivial insulator to TCI with the change of Sn content and temperature. Meanwhile, the surface states properties of Pb(1-x)Sn(x)Te are strongly dependent on crystallographic plane orientation. In this work, we first reported controllable synthesis of rectangular prismatic Pb(x)Sn(1-x)Te nanowires by vapor deposition method. Rectangular prismatic Pb(x)Sn(1-x)Te nanowires exhibits distinct {100} surfaces. Furthermore, The Sn composition of Pb(1-x)Sn(x)Te nanowires can be continuously controlled from 0 to 1. Low temperature magnetotransport shows that PbTe nanowire exhibits weak localization (WL) effect, whereas Pb0.5Sn0.5Te and Pb0.2Sn0.8Te nanowires display pronounced weak antilocalization (WAL) effect. This transition is explained by the topological phase transform of Pb(1-x)Sn(x)Te from trivial to nontrivial insulator with Sn content (x) exceeding 0.38. Pb(x)Sn(1-x)Te nanowires synthesized in this work lay a foundation for probing spin-correlated electron transport and show great potentials for future applications of tunable spintronic devices.
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Despite great progress in synthesis and application of graphene-like materials, it remains a considerable challenge to prepare two-dimensional (2D) nanostructures of nonlayered materials that may bring us surprising physical and chemical properties. Here, we propose a general strategy for the growth of 2D nonlayered materials by van der Waals epitaxy (vdWE) growth with two conditions: (1) the nonlayered materials satisfy 2D anisotropic growth and (2) the growth is implemented on the van der Waals substrates. Large-scale ultrathin 2D Pb(1-x)Sn(x)Se nanoplates (â¼15-45 nm) have been produced on mica sheets by applying this strategy. Benefiting from the 2D geometry of Pb(1-x)Sn(x)Se nanoplates and the flexibility of mica sheet, flexible photodetectors that exhibit fast, reversible, and stable photoresponse and broad spectra detection ranging from UV to infrared light (375, 473, 632, 800, and 980 nm) are in situ fabricated based on Pb(1-x)Sn(x)Se nanoplates. We anticipate that more nonlayered materials will be developed into 2D nanostructures through vdWE, enabling the exploitation of novel electronic and optoelectronic devices.
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Topological crystalline insulators (TCIs) are recently discovered topological phase with robust surface states residing on high-symmetry crystal surfaces. Different from conventional topological insulators (TIs), protection of surface states on TCIs comes from point-group symmetry instead of time-reversal symmetry in TIs. The distinct properties of TCIs make them promising candidates for the use in novel spintronics, low-dissipation quantum computation, tunable pressure sensor, mid-infrared detector, and thermoelectric conversion. However, similar to the situation in TIs, the surface states are always suppressed by bulk carriers, impeding the exploitation of topology-induced quantum phenomenon. One effective way to solve this problem is to grow low-dimensional TCIs which possess large surface-to-volume ratio, and thus profoundly increase the carrier contribution from topological surface states. Indeed, through persistent effort, researchers have obtained unique quantum transport phenomenon, originating from topological surface states, based on controllable growth of low-dimensional TCIs. This article gives a comprehensive review on the recent progress of controllable synthesis and topological surface transport of low-dimensional TCIs. The possible future direction about low-dimensional TCIs is also briefly discussed at the end of this paper.
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Surface states properties of topological crystalline insulator Pb1-x Snx Se are strongly dependent on crystallographic plane orientation. Rectangular prismatic Pbx Sn1-x Se nanowires and nanoplates are grown with distinct {100} surfaces on mica sheets. Substrate surface chemical properties are found to be the critical factors that affect the vapor deposition process and final shapes of Pb1-x Snx Se nanostructures.