Tunable Negative and Positive Photoconductance in Van Der Waals Heterostructure for Image Preprocessing.

The processing of visual information occurs mainly in the retina, and the retinal preprocessing function greatly improves the transmission quality and efficiency of visual information. The artificial retina system provides a promising path to efficient image processing. Here, graphene/InSe/h-BN heterogeneous structure is proposed, which exhibits negative and positive photoconductance (NPC and PPC) effects by altering the strength of a single wavelength laser. Moreover, a modified theoretical model is presented based on the power-dependent photoconductivity effect of laser: I ph = - mP α 1 + nP α 2 ${\rm I}_{\rm ph}\,=\,-{\rm mP}^{\alpha _{1}} + {\rm nP}^{\alpha _{2}}$ , which can reveal the internal physical mechanism of negative/positive photoconductance effects. The present 2D structure design allows the field effect transistor (FET) to exhibit excellent photoelectric performance (RNPC = 1.1× 104 AW-1, RPPC = 13 AW-1) and performance stability. Especially, the retinal pretreatment process is successfully simulated based on the negative and positive photoconductive effects. Moreover, the pulse signal input improves the device responsivity by 167%, and the transmission quality and efficiency of the visual signal can also be enhanced. This work provides a new design idea and direction for the construction of artificial vision, and lay a foundation for the integration of the next generation of optoelectronic devices.

Phase transition in WSe2-xTex monolayers driven by charge injection and pressure: a first-principles study.

Alloying strategies permit new probes for governing structural stability and semiconductor-semimetal phase transition of transition metal dichalcogenides (TMDs). However, the possible structure and phase transition mechanism of the alloy TMDs, and the effect of an external field, have been still unclear. Here, the enrichment of the Te content in WSe2-xTex monolayers allows for coherent structural transition from the H phase to the T' phase. The crystal orbital Hamiltonian population (COHP) uncovers that the bonding state of the H phase approaches the high-energy domain near the Fermi level as the Te concentration increases, posing a source of structural instability followed by a weakened energy barrier for the phase transition. In addition, the structural phase transition driven by charge injection opens up new possibilities for the development of phase-change devices based on atomic thin films. For WSe2-xTex monolayers with the H phase as the stable phase, the critical value of electron concentration triggering the phase transition decreases with an increase in the x value. Furthermore, the energy barrier from the H phase to the T' phase can be effectively reduced by applying tensile strain, which could favor the phase switching in electronic devices. This work provides a critical reference for controllable modulation of phase-sensitive devices from alloy materials with rich phase characteristics.

Correction: Silver/silver halide supported on mesoporous ceria particles and photo-CWPO degradation under visible light for organic compounds in acrylonitrile wastewater.

[This corrects the article DOI: 10.1039/D1RA04465F.].

A polar-switchable and controllable negative phototransistor for information encryption.

Anomalous negative phototransistors have emerged as a distinct research area, characterized by a decrease in channel current under light illumination. Recently, their potential applications have been expanded beyond photodetection. Despite the considerable attention given to negative phototransistors, negative photoconductance (NPC) in particular remains relatively unexplored, with limited research advancements as compared to well-established positive phototransistors. In this study, we designed ferroelectric field-effect transistors (FeFETs) based on the WSe2/CIPS van der Waals (vdW) vertical heterostructures with a buried-gated architecture. The transistor exhibits NPC and positive photoconductance (PPC), demonstrating the significant role of ferroelectric polarization in the distinctive photoresponse. The observed inverse photoconductance can be attributed to the dynamic switching of ferroelectric polarization and interfacial charge transfer processes, which have been investigated experimentally and theoretically using Density Functional Theory (DFT). The unique phenomena enable the coexistence of controllable and polarity-switchable PPC and NPC. The novel feature holds tremendous potential for applications in optical encryption, where the specific gate voltages and light can serve as universal keys to achieve modulation of conductivity. The ability to manipulate conductivity in response to optical stimuli opens up new avenues for developing secure communication systems and data storage technologies. Harnessing this feature enables the design of advanced encryption schemes that rely on the unique properties of our material system. The study not only advances the development of NPC but also paves the way for more robust and efficient methods of optical encryption, ensuring the confidentiality and integrity of critical information in various domains, including data transmission, and information security.

Optically Induced Multistage Phase Transition in Coherent Phonon-Dominated a-GeTe.

Ultrafast photoexcitation can decouple the multilevel nonequilibrium dynamics of electron-lattice interactions, providing an ideal probe for dissecting photoinduced phase transition in solids. Here, real-time time-dependent density functional theory simulations combined with occupation-constrained DFT methods are employed to explore the nonadiabatic paths of optically excited a-GeTe. Results show that the short-wavelength ultrafast laser is capable of generating full-domain carrier excitation and repopulation, whereas the long-wavelength ultrafast laser favors the excitation of lone pair electrons in the antibonded state. Photodoping makes the double-valley potential energy surface shallower and allows the insertion of A1g coherent forces in the atomic pairs, by which the phase reversal of Ge and Te atoms in the ⟨001⟩ direction is activated with ultrafast suppression of the Peierls distortion. These findings have far-reaching implications regarding nonequilibrium phase engineering strategies based on phase-change materials.

Directly measuring flexoelectric coefficients µ11 of the van der Waals materials.

Flexoelectricity originates from the electromechanical coupling interaction between strain gradient and polarization, broadly applied in developing electromechanical and energy devices. However, the study of quantifying the longitudinal flexoelectric coefficient (µ11) which is important for the application of atomic-scale two-dimensional (2D) materials is still in a slow-moving stage, owing to the technical challenges. Based on the free-standing suspension structure, this paper proposes a widely applicable method and a mensurable formula for determining the µ11 constant of layer-dependent 2D materials with high precision. A combination of in situ micro-Raman spectroscopy and piezoresponse force microscopy (PFM) imaging was used to quantify the strain distribution and effective out-of-plane electromechanical coupling, respectively, for µ11 constant calculation. The µ11 constants and their physical correlation with the variable mechanical conditions of naturally bent structures have been obtained extensively for the representative mono-to-few layered MX2 family (M = W and Mo; X = S and Se), and the result is perfectly consistent with the estimated order-of-magnitude of the µ11 value (about 0.065) of monolayer MoS2. The quantification of the flexoelectric constant in this work not only promotes the understanding of mechanical and electromechanical properties in van der Waals materials, but also paves the way for developing novel 2D nano-energy devices and mechanical transducers based on flexoelectric effects.

Tunable lattice dynamics and dielectric functions of two-dimensional Bi2O2Se: striking layer and temperature dependent effects.

Two-dimensional (2D) Bi2O2Se semiconductors with a narrow band gap and ultrahigh mobility have been regarded as an emerging candidate for optoelectronic devices, whereas the ambiguous phonon characteristics and optical properties still limit their future applications. Herein, high-quality centimeter-scale 2D Bi2O2Se films are successfully synthesized to disclose the lattice dynamics and dielectric functions under the control of thickness and temperature. It has been demonstrated that the stronger electrostatic Bi-Se interactions result in a stiffened phonon vibration of thicker Bi2O2Se layers. Three excitons (Ea, Eb, and Ec) exhibit significant red shifts with layer stacking. Interestingly, the dielectric properties in the visible-near infrared region (Ea and Eb) are dominated by the combined effect of the joint density of states and mass density, whereas the dielectric properties in the ultraviolet region (Ec) are dominated by the exciton effect. Furthermore, the temperature-sensitivity of the phonon frequency and exciton transition energies is revealed to be layer-dependent. In particular, the optical response of Eb excitons exhibits a prominent dependence on temperature, which indicates a promising optical modulation by temperature in the visible spectrum. This study enriches the knowledge about phonon dynamics and dielectric properties for 2D Bi2O2Se, which provides an essential reference for high-performance related optoelectronic devices.

Ultrathin Fe-ReS2 Nanosheets as Electrocatalysts for Accelerating Sulfur Reduction in Li-S Batteries.

Lithium-sulfur batteries are promising next-generation energy storage systems with high theoretical specific capacity. Despite extensive research efforts, it is still challenging to rationally design electrocatalysts with fast kinetics and effective adsorption of polysulfides. Herein, Fe-doped ReS2 (Fe-ReS2) ultrathin nanosheets are prepared as an electrocatalyst to trap the intermediates and accelerate the sulfur reduction reaction kinetics. Density functional theory calculations combined with activation energies in the multistep sulfur reduction reaction reveal that the Fe-ReS2 considerably reduces the activation energy and optimizes the optimum adsorption strength of polysulfides and catalytic activity. The Fe-ReS2/S exhibits a highly reversible discharge capacity of 882.3 mA h g-1 at 1 C. For 500 cycles, the capacity fade rate is 0.013% per cycle. Moreover, in situ Raman spectroscopy measurements further confirmed that both sulfur reduction and oxidation processes were significantly enhanced by Fe-ReS2.

Ultra-Stable, Endurable, and Flexible Sb2TexSe3-x Phase Change Devices for Memory Application and Wearable Electronics.

Flexible memory and wearable electronics represent an emerging technology, thanks to their reliability, compatibility, and superior performance. Here, an Sb2TexSe3-x (STSe) phase change material was grown on flexible mica, which not only exhibited superior nature in thermal stability for phase change memory application but also revealed novel function performance in wearable electronics, thanks to its excellent mechanical reliability and endurance. The thermal stability of Sb2Te3 was improved obviously with the crystallization temperature elevated 60 K after Se doping, for the enhanced charge localization and stronger bonding energy, which was validated by the Vienna ab initio simulation package calculations. Based on the ultra-stability of STSe, the STSe-based phase change memory shows 65 000 reversible phase change ability. Moreover, the assembled flexible device can show real-time monitoring and recoverability response in sensing human activities in different parts of the body, which proves its effective reusability and potential as wearable electronics. Most importantly, the STSe device presents remarkable working reliability, reflected by excellent endurance over 100 s and long retention over 100 h. These results paved a novel way to utilize STSe phase change materials for flexible memory and wearable electronics with extreme thermal and mechanical stability and brilliant performance.

Designing Monoclinic Heterophase Coexistence for the Enhanced Piezoelectric Performance in Ternary Lead-Based Relaxor Ferroelectrics.

Enhanced piezoelectric, dielectric properties and thermal stability in ternary relaxor-PbTiO3 based ferroelectric crystals are expected to develop the next-generation of electromechanical devices. However, due to their increased disorder compared to other ferroelectrics, designing a controllable phase boundary structure and engineered domain remains a challenging task. Here, we construct a monoclinic heterophase coexisting in a ternary Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 single crystal with optimized composition and an ultrahigh piezoelectric coefficient of 1400 pC N-1, to quantify the correlation between spontaneous nanopolarity and phase heterogeneity, in an attempt to understand the origin of the exceptional functionalities. By designing an in situ high-resolution spectroscopic-microscopic technique, we have observed Ma and Mc heterophase mixtures spatially separated by the monoclinic heterophase boundary (MHB), which are responsible for the ferroelectric-dominated and relaxor-ferroelectric-dominated nanodomain structure, respectively. Internal energy mapping from optical soft mode dynamics reveals the inhomogeneous polarization and local symmetry on both sides of the MHB. Various molecular polarizabilities and localized octahedral distortions correlate directly with monoclinic regions and electromechanical contribution. This work clarifies the heterogeneity between structure, energy, and polar order and provides a new design freedom for advanced relaxor ferroelectrics.

Ultrabroadband Tellurium Photoelectric Detector from Visible to Millimeter Wave.

Ultrabroadband photodetection is of great significance in numerous cutting-edge technologies including imaging, communications, and medicine. However, since photon detectors are selective in wavelength and thermal detectors are slow in response, developing high performance and ultrabroadband photodetectors is extremely difficult. Herein, one demonstrates an ultrabroadband photoelectric detector covering visible, infrared, terahertz, and millimeter wave simultaneously based on single metal-Te-metal structure. Through the two kinds of photoelectric effect synergy of photoexcited electron-hole pairs and electromagnetic induced well effect, the detector achieves the responsivities of 0.793 A W-1 at 635 nm, 9.38 A W-1 at 1550 nm, 9.83 A W-1 at 0.305 THz, 24.8 A W-1 at 0.250 THz, 87.8 A W-1 at 0.172 THz, and 986 A W-1 at 0.022 THz, respectively. It also exhibits excellent polarization detection with a dichroic ratio of 468. The excellent performance of the detector is further verified by high-resolution imaging experiments. Finally, the high stability of the detector is tested by long-term deposition in air and high-temperature aging. The strategy provides a recipe to achieve ultrabroadband photodetection with high sensitivity and fast response utilizing full photoelectric effect.

Thermal Conductivity of Large-Area Polycrystalline MoSe2 Films Grown by Chemical Vapor Deposition.

It is of great importance to understand the thermal properties of MoSe2 films for electronic and optoelectronic applications. In this work, large-area polycrystalline MoSe2 films are prepared using a low-cost, controllable, large-scale, and repeatable chemical vapor deposition method, which facilitates direct device fabrication. Raman spectra and X-ray diffraction patterns indicate a hexagonal (2H) crystal structure of the MoSe2 film. Ellipsometric spectra analysis indicates that the optical band gap of the MoSe2 film is estimated to be ∼1.23 eV. From the analysis of the temperature-dependent and laser-power-dependent Raman spectra, the thermal conductivity of the suspended MoSe2 films is found to be ∼28.48 W/(m·K) at room temperature. The results can provide useful guidance for an effective thermal management of large-area polycrystalline MoSe2-based electronic and optoelectronic devices.

Flexo-photoelectronic effect in n-type/p-type two-dimensional semiconductors and a deriving light-stimulated artificial synapse.

Flexoelectricity and photoelectricity with their coupled effect (the so-called flexo-photoelectronic effect), are of increasing interest in the study of electronics and optoelectronics in van der Waals layered semiconductors. However, the related device design is severely restricted owing to the ambiguous underlying physical nature of flexo-photoelectronic effects originating from the co-manipulation of light and strain-gradients. Here, flexoelectric polarization and the flexo-photoelectronic effect of few-layered semiconductors have been multi-dimensionally investigated from high-resolution microscopic characterization on the nanoscale, physics analysis, and deriving a device design. We found that two back-to-back built-in electric fields form in bent InSe and WSe2, and greatly modulate the transport behaviors of photogenerated carriers, further facilitating the separation of photogenerated electron-hole pairs and trapping the holes/electrons in InSe or WSe2 channels, recorded in realtime by a home-made technique of lighting Kelvin probe force microscopy (KPFM). The slow release of trapped carriers contributes to the photoconductance relaxation after illumination. Utilizing the photoconductance relaxation, a light-stimulated artificial synapse based on the flexo-photoelectronic effect of bent InSe has been achieved. Significantly, all the pair-pulse facilitation (PPF) behavior, spike frequency-dependent excitatory post-synaptic current (EPSC) and the transition from short-term memory (STM) to long-term memory (LTM) have been successfully realized in this artificial synapse. This work adds to the investigation of flexo-photoelectronic effects on 2D optoelectronics, and moves towards the development of 2D neuromorphic electronics.

Optically Modulated HfS2-Based Synapses for Artificial Vision Systems.

The simulation of human brain neurons by synaptic devices could be an effective strategy to break through the notorious "von Neumann Bottleneck" and "Memory Wall". Herein, opto-electronic synapses based on layered hafnium disulfide (HfS2) transistors have been investigated. The basic functions of biological synapses are realized and optimized by modifying pulsed light conditions. Furthermore, 2 × 2 pixel imaging chips have also been developed. Two-pixel visual information is illuminated on diagonal pixels of the imaging array by applying light pulses (λ = 405 nm) with different pulse frequencies, mimicking short-term memory and long-term memory characteristics of the human vision system. In addition, an optically/electrically driven neuromorphic computation is demonstrated by machine learning to classify hand-written numbers with an accuracy of about 88.5%. This work will be an important step toward an artificial neural network comprising neuromorphic vision sensing and training functions.

Silver/silver halide supported on mesoporous ceria particles and photo-CWPO degradation under visible light for organic compounds in acrylonitrile wastewater.

Silver/silver halide supported on ordered mesoporous ceria particles (Ag/AgCl/CeO2) were rapidly prepared by microwave-assisted soft template method, deposition precipitation method and photoreduction method, using cerium nitrate and silver nitrate as raw materials and block copolymer F127 as a template. The morphology, structure and chemical composition of the catalyst were characterized by XRD, SEM, EDS, TEM, N2 adsorption-desorption and UV-Vis Drs. Catalytic wet peroxide system assisted with visible light photocatalysis (photo-CWPO) was conducted to investigate the performance of organics degradation by Ag/AgCl/CeO2 as a catalyst in acrylonitrile wastewater. The results showed that the Ag/AgCl/CeO2 prepared has an ordered mesoporous structure, Ag and AgCl are formed on the surface of CeO2, with a specific surface area of 302.6-336.2 m2 g-1 and the average pore size is 8.04-8.90 nm. There is a strong absorption in the visible region and a band gap of 2.9 eV. The Ag/AgCl/CeO2 catalyst has higher catalytic performance in the photo-CWPO system than in the CWPO system alone. Ag loading, catalyst and H2O2 dosage, and pH value can affect the COD removal. When the concentration of COD in acrylonitrile wastewater was 500 mg L-1, the amount of catalyst was 200 mg, the amount of H2O2 (30%) was 8 mL, and the reaction time was 60 min, the COD removal reached 90%.

Ferroelectric-Modulated MoS2 Field-Effect Transistors as Multilevel Nonvolatile Memory.

Ferroelectric field-effect transistors (FeFETs) with semiconductors as the channel material and ferroelectrics as the gate insulator are attractive and/or promising devices for application in nonvolatile memory. In FeFETs, the conductivity states of the semiconductor are utilized to explore the polarization directions of the ferroelectric material. Herein, we report FeFETs based on a few layers of MoS2 on a 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (PMN-PT) single crystal with switchable multilevel states. It was found that the On-Off ratios can reach as high as 106. We prove that the interaction effect of ferroelectric polarization and interface charge traps has a great influence on the transport behaviors and nonvolatile memory characteristics of MoS2/PMN-PT FeFETs. In order to further study the underlying physical mechanism, we have researched the time-dependent electrical properties in the temperature range from 300 to 500 K. The separation of effects from ferroelectric polarization and interfacial traps on electrical behaviors of FeFETs provides us with an opportunity to better understand the operation mechanism, which suggests a fantastic way for multilevel, low-power consumption, and high-density nonvolatile memory devices.

P-N conversion of charge carrier types and high photoresponsive performance of composition modulated ternary alloy W(SxSe1-x)2 field-effect transistors.

Transition metal dichalcogenides (TMDs) have emerged as a new class of two-dimensional (2D) materials, which are promising for diverse applications in nanoelectronics, optoelectronics, and photonics. To satisfy the requirements of the building blocks of functional devices, systematic modulation of the band gap and carrier type of TMDs materials becomes a significant challenge. Here, we report a salt-assisted chemical vapor deposition (CVD) approach for the simultaneous growth of alloy W(SxSe1-x)2 nanosheets with variable alloy compositions. Electrical transport studies based on the as-fabricated W(SxSe1-x)2 nanosheet field-effect transistors (FETs) demonstrate that charge carrier types of alloy nanosheet transistors can be systematically tuned by adjusting the alloy composition. Temperature-dependent current measurement shows that the main scattering mechanism is the charged impurity scattering. The effective Schottky barrier heights of bipolar W(SxSe1-x)2 transistors are initially increased and then decreased with increasing positive (or negative) gate voltage, which is tunable by varying the alloy composition. In addition, the tunability of these W(SxSe1-x)2-based ambipolar transistors is suitable for logic and analog applications and represents a critical step toward future fundamental studies as well as for the rational design of new 2D electronics with tailored spectral responses, and simpler and higher integration densities. Finally, the high photoresponsivity (up to 914 mA W-1) and detectivity (4.57 × 1010 Jones) of ultrathin W(SxSe1-x)2 phototransistors imply their potential applications in flexible light-detection and light-harvesting devices. These band gap engineered 2D structures could open up an exciting opportunity and contribute to finding diverse applications in future functional electronic/optoelectronic devices.

Roles for heterodimerization of APJ and B2R in promoting cell proliferation via ERK1/2-eNOS signaling pathway.

Apelin receptor (APJ) and bradykinin B2 receptor (B2R) play an important role in many physiological processes and share multiple similar characteristics in distribution and functions in the cardiovascular system. We first identified the endogenous expression of APJ and B2R in human umbilical vein endothelial cells (HUVECs) and their co-localization on human embryonic kidney (HEK) 293 cells membrane. A suite of bioluminescence and fluorescence resonance energy transfer (BRET and FRET), proximity ligation assay (PLA), and co-immunoprecipitation (Co-IP) was exploited to demonstrate formation of functional APJ and B2R heterodimer in HUVECs and transfected cells. Stimulation with apelin-13 and bradykinin (BK) increased the phosphorylation of the endothelial nitric oxide synthase (eNOS) in HUVECs, which could be inhibited by the silencing of APJ or B2R, indicating the APJ-B2R dimer is critical for eNOS phosphorylation in HUVECs. Furthermore, the increase of NOS and extracellular signal regulated kinases1/2 (ERK1/2) phosphorylation mediated by APJ/B2R dimer can be inhibited by U0126 and U73122, respectively, suggesting that the heterodimer might activate the PLC/ERK1/2/eNOS signaling pathway, and finally leading to a significant increase in cell proliferation. Thus, we uncovered for the first time the existence of APJ-B2R heterodimer and provided a promising new target in cardiovascular therapeutics.

Superior and Reversible Lithium Storage of SnO2/Graphene Composites by Silicon Doping and Carbon Sealing.

The poor cycle stability and reversibility seriously hinder the widespread application of SnO2 materials as anodes for lithium-ion batteries (LIBs). A novel sandwich-architecture composite of Si-doped SnO2 nanorods and reduced graphene oxide with carbon sealing (Si-SnO2@G@C) is engineered and fabricated by a facile two-step hydrothermal process and subsequent annealing treatment, which exhibit not only extraordinary rate performance and ultrahigh reversible capacity but also excellent cycle stability and high electrical conductivity as the anode of LIBs. The Si-doped SnO2 nanoparticles on the surface of graphene were firmly wrapped in the C-coating and formed a porous sandwich structure, which can efficiently prevent the Sn nanoparticles from aggregation and provide more extra space for accommodating the volume variations and more active sites for reactions. The carbon layer also blocks the direct contact of the SnO2 nanorods with electrolyte and prevents the graphene nanosheets from the restacking. More importantly, the reversibility of lithiation/delithiation reactions can be remarkably improved by the doping silicon. The doped Si not only accelerates the diffusion of Li+ but also brings a significant increase in the specific capacity. As a consequence, the Si-SnO2@G@C nanocomposite can maintain a high capacity of 654 mAh/g at 2 A/g even after 1200 cycles with negligible capacity loss and excellent reversibility with a Coulombic efficiency retention over 99%, which can be capable of the alternative to commercial graphite anodes. This work provides a new strategy for the reasonable design of advanced anode materials with superior and reversible lithium storage capacity.

Mixed-Dimensional Van der Waals Heterostructure Photodetector.

Van der Waals (vdW) heterostructures, integrated two-dimensional (2D) materials with various functional materials, provide a distinctive platform for next-generation optoelectronics with unique flexibility and high performance. However, exploring the vdW heterostructures combined with strongly correlated electronic materials is hitherto rare. Herein, a novel temperature-sensitive photodetector based on the GaSe/VO2 mixed-dimensional vdW heterostructure is discovered. Compared with previous devices, our photodetector exhibits excellent enhanced performance, with an external quantum efficiency of up to 109.6% and the highest responsivity (358.1 mA·W-1) under a 405 nm laser. Interestingly, we show that the heterostructure overcomes the limitation of a single material under the interaction between VO2 and GaSe, where the photoresponse is highly sensitive to temperature and can be further vanished at the critical value. The metal-insulator transition of VO2, which controls the peculiar band-structure evolution across the heterointerface, is demonstrated to manipulate the photoresponse variation. This study enables us to elucidate the method of manipulating 2D materials by strongly correlated electronic materials, paving the way for developing high-performance and special optoelectronic applications.