RESUMO
With the ability to maximize the exposure of nearly all active sites to reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class of materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding of catalytic behaviors at a single material level, significantly promoting this field. This Review provides an overview of the recent progress in microcell-based TMD electrocatalyst studies. We first introduced the structural characteristics of TMD materials and discussed their site engineering strategies for electrocatalysis. Later, we comprehensively described two distinct types of microcells: the window-confined on-chip electrochemical microcell (OCEM) and the droplet-confined scanning electrochemical cell microscopy (SECCM). Their setups, working principles, and instrumentation were elucidated in detail, respectively. Furthermore, we summarized recent advances of OCEM and SECCM obtained in TMD catalysts, such as active site identification and imaging, site monitoring, modulation of charge injection and transport, and electrostatic field gating. Finally, we discussed the current challenges and provided personal perspectives on electrochemical microcell research.
RESUMO
FeTe1-xSex, a promising layered material used to realize Majorana zero modes, has attracted enormous attention in recent years. Pulsed laser deposition (PLD) and molecular-beam epitaxy (MBE) are the routine growth methods used to prepare FeTe1-xSex thin films. However, both methods require high-vacuum conditions and polished crystalline substrates, which hinder the exploration of the topological superconductivity and related nanodevices of this material. Here we demonstrate the growth of the ultrathin FeTe1-xSex superconductor by a facile, atmospheric pressure chemical vapor deposition (CVD) method. The composition and thickness of the two-dimensional (2D) FeTe1-xSex nanosheets are well controlled by tuning the experimental conditions. The as-prepared FeTe0.8Se0.2 nanosheet exhibits an onset superconducting transition temperature of 12.4 K, proving its high quality. Our work offers an effective strategy for preparing the ultrathin FeTe1-xSex superconductor, which could become a promising platform for further study of the unconventional superconductivity in the FeTe1-xSex system.
RESUMO
Transition metal dichalcogenides (TMDs) have become a playground for exploring rich physical phenomena like superconductivity and charge-density-waves (CDW). Here, we report the synthesis of the atom-thin TaSe2 with a rare 3R phase and enhanced superconductivity. The 3R phase is achieved by an ambient pressure chemical vapor deposition (CVD) strategy and confirmed by the high-resolution aberration-corrected STEM. Low-temperature transport data reveal an enhanced superconducting transition temperature (Tc) of 1.6 K in the 3R-TaSe2, which undoubtedly breaks the traditional perception of TaSe2 crystal as a material with Tc close to 0 K. This work demonstrates the strength of ambient pressure CVD in the exploration of crystal polymorphism, highlights a decisive role of layer stacking order in the superconducting transition, and provides fresh insights on manipulating crystal structures to gain access to enhanced Tc.
RESUMO
The metal-to-core charge transfer (MCCT) transition in sensitized titanium-oxo clusters is an important process for photoinduced electron injection in photovoltaic conversion. This process resembles most closely the Type II photoinjection in dye-sensitized solar cells. Herein we report the synthesis and photophysical and photoelectrochemical (PEC) properties of the phosphonate-stabilized titanium-oxo clusters containing the ferrocenecarboxylate ligands. These ferrocene-containing clusters exhibit intense visible absorption extended up to 600 nm along with low optical band gaps of â¼2.2 eV. The low-energy transitions of these clusters were systematically investigated by UV-vis spectroscopy and DFT/TDDFT calculations. The combined experimental and computational studies suggest that the ferrocenecarboxylate-substituted titanium-oxo clusters form a donor-acceptor (D-A) system. The low-energy transition of these clusters primarily involves the MCCT from the iron center to TiO cluster core. The TiO core structure and phosphonate ligands both have great influence on the PEC properties of the clusters. This work provides valuable examples for the sensitized titanium-oxo clusters in which electron injection takes place via MCCT transition.
RESUMO
The ambient stability is one of the focal points for applications of 2D materials, especially for those well-known air-sensitive ones, such as black phosphorus (BP) and transitional metal telluride. Traditional methods of encapsulation, such as atomic layer deposition of oxides and heterogeneous integration of hexagonal boron nitride, can hardly avoid removal of encapsulation layer when the 2D materials are encapsulated for further device fabrication, which causes complexity and damage during the procedure. Here, a van der Waals encapsulation method that allows direct device fabrication without removal of encapsulation layer is introduced using Ga2O3 from liquid gallium. Taking advantage of the robust isolation ability against ambient environment of the dense native oxide of gallium, hundreds of times longer retention time of (opto)electronic properties of encapsulated BP and MoTe2 devices is realized than unencapsulated devices. Due to the ultrathin high-κ properties of Ga2O3, top-gated devices are directly fabricated with the encapsulation layer, simultaneously as a dielectric layer. This direct device fabrication is realized by selective etching of Ga2O3, leaving the encapsulated materials intact. Encapsulated 1T' MoTe2 exhibits high conductivity even after 150 days in ambient environment. This method is, therefore, highlighted as a promising and distinctive one compared with traditional passivation approaches.
RESUMO
A light field carrying multidimensional optical information, including but not limited to polarization, intensity and wavelength, is essential for numerous applications such as environmental monitoring, thermal imaging, medical diagnosis and free-space communications. Simultaneous acquisition of this multidimensional information could provide comprehensive insights for understanding complex environments but remains a challenge. Here we demonstrate a multidimensional optical information detection device based on zero-bias double twisted black arsenic-phosphorus homojunctions, where the photoresponse is dominated by the photothermoelectric effect. By using a bipolar and phase-offset polarization photoresponse, the device operated in the mid-infrared range can simultaneously detect both the polarization angle and incident intensity information through direct measurement of the photocurrents in the double twisted black arsenic-phosphorus homojunctions. The device's responsivity makes it possible to retrieve wavelength information, typically perceived as difficult to obtain. Moreover, the device exhibits an electrically tunable polarization photoresponse, enabling precise distinction of polarization angles under low-intensity light exposure. These demonstrations offer a promising approach for simultaneous detection of multidimensional optical information, indicating potential for diverse photonic applications.
RESUMO
Spin-polarized bands in pristine and proximity-induced magnetic materials are promising building blocks for future devices. Conceptually new memory, logic, and neuromorphic devices are conceived based on atomically thin magnetic materials and the manipulation of their spin-polarized bands via electrical and optical methods. A critical remaining issue is the direct probe and the optimized use of the magnetic coupling effect in van der Waals heterostructures, which requires further delicate design of atomically thin magnetic materials and devices. Here, a spin-selective memtransistor with magnetized single-layered graphene on a reactive antiferromagnetic material, CrI3, is reported. The spin-dependent hybridization between graphene and CrI3 atomic layers enables the spin-selective bandgap opening in the single-layered graphene and the electric field control of magnetization in a specific CrI3 layer. The microscopic working principle is clarified by the first-principles calculations and theoretical analysis of the transport data. Reliable memtransistor operations (i.e., memory and logic device-combined operations), as well as a spin-selective probe of Landau levels in the magnetized graphene, are achieved by using the subtle manipulation of the magnetic proximity effect via electrical means.
RESUMO
Nonlinear optical activities, especially second harmonic generation (SHG), are key phenomena in inversion-symmetry-broken two-dimensional (2D) transition metal dichalcogenides (TMDCs). On the other hand, anisotropic nonlinear optical processes are important for unique applications in nano-nonlinear photonic devices with polarization functions, having become one of focused research topics in the field of nonlinear photonics. However, the strong nonlinearity and strong optical anisotropy do not exist simultaneously in common 2D materials. Here, we demonstrate strong second-order and third-order susceptibilities of 64 pm/V and 6.2×10-19 m2/V2, respectively, in the even-layer PdPSe, which has not been discovered in other common TMDCs (e.g., MoS2). Strikingly, it also simultaneously exhibited strong SHG anisotropy with an anisotropic ratio of ~45, which is the largest reported among all 2D materials to date, to the best of our knowledge. In addition, the SHG anisotropy ratio can be harnessed from 0.12 to 45 (375 times) by varying the excitation wavelength due to the dispersion of χ ( 2 ) values. As an illustrative example, we further demonstrate polarized SHG imaging for potential applications in crystal orientation identification and polarization-dependent spatial encoding. These findings in 2D PdPSe are promising for nonlinear nanophotonic and optoelectronic applications.
RESUMO
Two-dimensional ultrathin ferroelectrics have attracted much interest due to their potential application in high-density integration of non-volatile memory devices. Recently, 2D van der Waals ferroelectric based on interlayer translation has been reported in twisted bilayer h-BN and transition metal dichalcogenides (TMDs). However, sliding ferroelectricity is not well studied in non-twisted homo-bilayer TMD grown directly by chemical vapor deposition (CVD). In this paper, for the first time, experimental observation of a room-temperature out-of-plane ferroelectric switch in semiconducting bilayer 3R MoS2 synthesized by reverse-flow CVD is reported. Piezoelectric force microscopy (PFM) hysteretic loops and first principle calculations demonstrate that the ferroelectric nature and polarization switching processes are based on interlayer sliding. The vertical Au/3R MoS2/Pt device exhibits a switchable diode effect. Polarization modulated Schottky barrier height and polarization coupling of interfacial deep states trapping/detrapping may serve in coordination to determine switchable diode effect. The room-temperature ferroelectricity of CVD-grown MoS2 will proceed with the potential wafer-scale integration of 2D TMDs in the logic circuit.
RESUMO
The development of new near-infrared-responsive photocatalysts is a fascinating and challenging approach to acquire high photocatalytic hydrogen evolution (PHE) performance. Herein, near-infrared-responsive black CuVP2S6 and CuCrP2S6 flakes, as well as CuInP2S6 flakes, are designed and constructed for PHE. Atom-resolved scanning transmission electron microscopy images and X-ray absorption fine structure evidence the formation of ultrathin single-crystalline sheet-like structure of CuVP2S6 and CuCrP2S6. The synthetic CuVP2S6 and CuCrP2S6, with a narrow bandgap of ≈1.0 eV, shows the high light-absorption edge exceeding 1100 nm. Moreover, through the femtosecond-resolved transient absorption spectroscopy, CuCrP2S6 displays the efficient charge transfer and long charge lifetime (18318.1 ps), which is nearly 3 and 29 times longer than that of CuVP2S6 and CuInP2S6, respectively. In addition, CuCrP2S6, with the appropriate d-band and p-band, is thermodynamically favorable for the H+ adsorption and H2 desorption by contrast with CuVP2S6 and CuInP2S6. As a result, CuCrP2S6 exhibits high PHE rates of 9.12 and 0.66 mmol h-1 g-1 under simulated sunlight and near-infrared light irradiation, respectively, far exceeding other layered metal phospho-sulfides. This work offers a distinctive perspective for the development of new near-infrared-responsive photocatalysts.
RESUMO
2D materials are burgeoning as promising candidates for investigating nonlinear optical effects due to high nonlinear susceptibilities, broadband optical response, and tunable nonlinearity. However, most 2D materials suffer from poor nonlinear conversion efficiencies, resulting from reduced light-matter interactions and lack of phase matching at atomic thicknesses. Herein, a new 2D nonlinear material, niobium oxide dibromide (NbOBr2) is reported, featuring strong and anisotropic optical nonlinearities with scalable nonlinear intensity. Furthermore, Fabry-Pérot (F-P) microcavities are constructed by coupling NbOBr2 with air holes in silicon. Remarkable enhancement factors of ≈630 times in second harmonic generation (SHG) and 210 times in third harmonic generation (THG) are achieved on cavity at the resonance wavelength of 1500 nm. Notably, the cavity enhancement effect exhibits strong anisotropic feature tunable with pump wavelength, owing to the robust optical birefringence of NbOBr2. The ratio of the enhancement factor along the b- and c-axis of NbOBr2 reaches 2.43 and 5.27 for SHG and THG at 1500 nm pump, respectively, which leads to an extraordinarily high SHG anisotropic ratio of 17.82 and a 10° rotation of THG polarization. The research presents a feasible and practical strategy for developing high-efficiency and low-power-pumped on-chip nonlinear optical devices with tunable anisotropy.
RESUMO
The advent of 2D ferroelectrics, characterized by their spontaneous polarization states in layer-by-layer domains without the limitation of a finite size effect, brings enormous promise for applications in integrated optoelectronic devices. Comparing with semiconductor/insulator devices, ferroelectric devices show natural advantages such as non-volatility, low energy consumption and high response speed. Several 2D ferroelectric materials have been reported, however, the device implementation particularly for optoelectronic application remains largely hypothetical. Here, the linear electro-optic effect in 2D ferroelectrics is discovered and electrically tunable 2D ferroelectric metalens is demonstrated. The linear electric-field modulation of light is verified in 2D ferroelectric CuInP2S6. The in-plane phase retardation can be continuously tuned by a transverse DC electric field, yielding an effective electro-optic coefficient rc of 20.28 pm V-1. The CuInP2S6 crystal exhibits birefringence with the fast axis oriented along its (010) plane. The 2D ferroelectric Fresnel metalens shows efficacious focusing ability with an electrical modulation efficiency of the focusing exceeding 34%. The theoretical analysis uncovers the origin of the birefringence and unveil its ultralow light absorption across a wide wavelength range in this non-excitonic system. The van der Waals ferroelectrics enable room-temperature electrical modulation of light and offer the freedom of heterogeneous integration with silicon and another material system for highly compact and tunable photonics and metaoptics.
RESUMO
The presence of Escherichia coli (E. coli) in food and drinking water is a chronic problem worldwide. Protecting food against bacterial contamination and rapid diagnosis of infection require simple and rapid assays for detection of bacterial pathogens, including E. coli O157:H7. Here we report a rapid and novel colorimetric method for detecting E. coli O157:H7. This colorimetric method is based on the catalytic oxidation of the peroxidase substrate 3,3,5,5-tetramethylbenzidine by hydrogen peroxide using 4-mercaptophenylboronic acid-functioned Au@Pt nanoparticles adsorbed on the surface of E. coli O157:H7. The assay showed excellent sensitivity both with the naked eye and based on absorbance measurements. The absorbance at 652 nm was proportional to the concentration of E. coli O157:H7 ranging from 7 to 6 × 10(6) cfu mL(-1) with a limit of detection of 7 cfu mL(-1). The total detection time was less than 40 min.
Assuntos
Escherichia coli O157/isolamento & purificação , Ouro/química , Nanopartículas Metálicas/química , Peroxidase/química , Platina/química , Colorimetria , Peroxidase/metabolismoRESUMO
The emergence of van der Waals (vdW) heterostructures has led to precise and versatile methods of fabricating devices with atomic-scale accuracies. Hence, vdW heterostructures have shown much promise for technologies including photodetectors, photocatalysis, photovoltaic devices, ultrafast photonic devices, and field-effect transistors. These applications, however, remain confined to optical and suboptical regimes. Here, we theoretically show and experimentally demonstrate the use of vdW heterostructures as platforms for multicolor x-ray generation. By driving the vdW heterostructures with free electrons in a table-top setup, we generate x-ray photons whose output spectral profile can be user-customized via the heterostructure design and even controlled in real time. We show that the multicolor photon energies and their corresponding intensities can be tailored by varying the electron energy, the electron beam position, as well as the geometry and composition of the vdW heterostructure. Our results reveal the promise of vdW heterostructures in realizing highly versatile x-ray sources for emerging applications in advanced x-ray imaging and spectroscopy.
RESUMO
Nonlinear optical activities (e.g., harmonic generations) in two-dimensional (2D) layered materials have attracted much attention due to the great promise in diverse optoelectronic applications such as nonlinear optical modulators, nonreciprocal optical device, and nonlinear optical imaging. Exploration of nonlinear optical response (e.g., frequency conversion) in the infrared, especially the mid-infrared (MIR) region, is highly desirable for ultrafast MIR laser applications ranging from tunable MIR coherent sources, MIR supercontinuum generation, and MIR frequency-comb-based spectroscopy to high harmonic generation. However, nonlinear optical effects in 2D layered materials under MIR pump are rarely reported, mainly due to the lack of suitable 2D layered materials. Van der Waals layered platinum disulfide (PtS2) with a sizable bandgap from the visible to the infrared region is a promising candidate for realizing MIR nonlinear optical devices. In this work, we investigate the nonlinear optical properties including third-and fifth-harmonic generation (THG and FHG) in thin layered PtS2 under infrared pump (1550-2510 nm). Strikingly, the ultrastrong third-order nonlinear susceptibility χ(3)(-3ω;ω,ω,ω) of thin layered PtS2 in the MIR region was estimated to be over 10-18 m2/V2, which is about one order of that in traditional transition metal chalcogenides. Such excellent performance makes air-stable PtS2 a potential candidate for developing next-generation MIR nonlinear photonic devices.
RESUMO
Infrared machine vision system for object perception and recognition is becoming increasingly important in the Internet of Things era. However, the current system suffers from bulkiness and inefficiency as compared to the human retina with the intelligent and compact neural architecture. Here, we present a retina-inspired mid-infrared (MIR) optoelectronic device based on a two-dimensional (2D) heterostructure for simultaneous data perception and encoding. A single device can perceive the illumination intensity of a MIR stimulus signal, while encoding the intensity into a spike train based on a rate encoding algorithm for subsequent neuromorphic computing with the assistance of an all-optical excitation mechanism, a stochastic near-infrared (NIR) sampling terminal. The device features wide dynamic working range, high encoding precision, and flexible adaption ability to the MIR intensity. Moreover, an inference accuracy more than 96% to MIR MNIST data set encoded by the device is achieved using a trained spiking neural network (SNN).
RESUMO
Van der Waals (vdW) materials have attracted much interest for their myriad unique electronic, mechanical, and thermal properties. In particular, they are promising candidates for monochromatic, table-top X-ray sources. This work reveals that the versatility of the table-top vdW X-ray source goes beyond what has been demonstrated so far. By introducing a tilt angle between the vdW structure and the incident electron beam, it is theoretically and experimentally shown that the accessible photon energy range is more than doubled. This allows for greater versatility in real-time tuning of the vdW X-ray source. Furthermore, this work shows that the accessible photon energy range is maximized by simultaneously controlling both the electron energy and the vdW structure tilt. These results will pave the way for highly tunable, compact X-ray sources, with potential applications including hyperspectral X-ray fluoroscopy and X-ray quantum optics.
RESUMO
Defect states dominate the performance of low-dimensional nanoelectronics, which deteriorate the serviceability of devices in most cases. But in recent years, some intriguing functionalities are discovered by defect engineering. In this work, we demonstrate a bifunctional memory device of a MoS2/BiFeO3/SrTiO3 van der Waals heterostructure, which can be programmed and erased by solely one kind of external stimuli (light or electrical-gate pulse) via engineering of oxygen-vacancy-based solid-ionic gating. The device shows multibit electrical memory capability (>22 bits) with a large linearly tunable dynamic range of 7.1 × 106 (137 dB). Furthermore, the device can be programmed by green- and red-light illuminations and then erased by UV light pulses. Besides, the photoresponse under red-light illumination reaches a high photoresponsivity (6.7 × 104 A/W) and photodetectivity (2.12 × 1013 Jones). These results highlighted solid-ionic memory for building up multifunctional electronic and optoelectronic devices.
RESUMO
Transition metal tellurides (TMTs) have attracted intense interest due to their intriguing physical properties arising from their diverse phase topologies. To date, a wide range of physical properties have been discovered for TMTs, including that they can act as topological insulators, semiconductors, Weyl semimetals, and superconductors. Among the TMT families, MoTe2 is a representative material because of its Janus nature and rich phases. In this Perspective, we first introduce phase structures in monolayer and bulk MoTe2 and then summarize MoTe2 synthesis strategies. We highlight recent advances of Janus MoTe2 in terms of material structures and emerging quantum states. We also provide insight into the opportunities and challenges faced by MoTe2-associated device design and applications.
RESUMO
Excitons in monolayer transition metal dichalcogenides (TMDs) provide a paradigm of composite Boson in a two-dimensional system. This Letter reports a photoluminescence and reflectance study of excitons in monolayer molybdenum diselenide (MoSe2) with electrostatic gating. We observe the repulsive and attractive Fermi polaron modes of the band edge exciton, its excited state, and the spin-off excitons, which the simple three-particle trion model is insufficient to explain. The contrasting energy shift between the exciton and charge-bound excitons (repulsive and attractive polaron modes) and the remarkably different gate dependence of the polaron energy splitting between the ground state and the excited state excitons unambiguously support the Fermi polaron picture for excitons in monolayer TMDs.