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Scanning ion conductance microscopy (SICM) is a powerful surface imaging tool used in the electrolytic environment. Tip-enhanced Raman spectroscopy (TERS) can give more information in addition to the morphology provided by the SICM by utilizing label-free Raman spectroscopy aided by the localized plasmonic enhancement from the metal-coated probes. In this study, the integration of SICM with TERS is demonstrated through employing a silver-coated plasmonic nanopipette. Leveraging a two-dimensional (2D) molybdenum disulfide (MoS 2 ) as a model system, the SICM-TERS enhancement factor was estimated to be ∼10 5 , supported by finite-difference time-domain (FDTD) simulation. Moreover, the subnanometer distance dependence SICM-TERS study reveals the tensile stress and structural changes caused by the nanopipette. These findings illustrate the potential of SICM-TERS for providing comprehensive morphological and chemical insights into electrolytic environments, paving the way for future investigations of electrocatalytic and biological systems.

Artificial ionic sensory systems, bridging the divide between biological systems and electronics, mimic human skin functions but face critical challenges with biocompatibility, comfort, signal stability, and simplifying packaging. Here, we present a simple and permeable skin-interfaced iontronic mechanosensing (SIIM) architecture that integrates human skin as natural ionic material and hierarchically porous MXene-fiber composite membranes as sensing electrodes. The SIIM system eliminates complex ionic material design and multilayer matrix, exhibiting ultrahigh pressure sensitivities (5.4 kPa -1 , <75 Pa), a low detection limit (6 Pa), excellent output stability along with high permeability to minimize the impact of sweating on sensing. The noncytotoxic nature of SIIM electrodes ensures excellent biocompatibility (>97% cell coincubational viability), facilitating long-term wearability and high biosafety. Furthermore, the scalable SIIM configuration integrated with matrix smart gloves, effectively monitors human physical movements. This SIIM-based sensor with marked sensing capabilities, structural simplicity, and scalability, holds promising potential in diverse wearable applications.

Transition metal dichalcogenides (TMDCs) are at the forefront of nanophotonics because of their exceptional optical characteristics. The 2D architecture of TMDCs facilitates efficient light absorption and emission, holding tantalizing potential for next-generation nanophotonic and quantum devices. Yet, the atomic thinness limits their interaction volume with light, affecting light-matter interaction and quantum efficiency. The light coupling in the 2D layered TMDCs can be enhanced by integration with photonic structure, and the metasurfaces supporting bound states in the continuum (BICs) offer strong confinement of optical fields, ideal for coupling with 2D TMDCs. Here, we demonstrate enhanced light-matter coupling by integrating TMDC monolayers, including WSe 2 and MoS 2 , with a finite-area membrane metasurface, leading to amplified and high-quality-factor ( Q -factor) spontaneous emission from quasi-BIC-coupled TMDC monolayers. The high- Q -factor emission extends over an area with a scale of a few micrometers while maintaining the high- Q factor across the emission area. Notably, the suspended finite-area membrane metasurface, which is freestanding in air rather than positioned atop a substrate, minimizes radiation loss while enhancing light-matter interaction in the TMDC monolayer. Furthermore, the predominantly in-plane dipole orientation of excitons within TMDC monolayers results in distinctive enhancement behaviors for emission, contingent on the excitation power, when coupled with quasi-BIC modes exhibiting TE and TM resonances. This work introduces a nanophotonic platform for robust coupling of membrane metasurfaces with 2D materials, offering possibilities for developing 2D material-based nanophotonic and quantum devices.

Atomically thin 2D films and their van der Waals heterostructures have demonstrated immense potential for breakthroughs and innovations in science and technology. Integrating 2D films into electronics and optoelectronics devices and their applications in electronics and optoelectronics can lead to improve device efficiencies and tunability. Consequently, there has been steady progress in large-area 2D films for both front- and back-end technologies, with a keen interest in optimizing different growth and synthetic techniques. Parallelly, a significant amount of attention has been directed toward efficient transfer techniques of 2D films on different substrates. Current methods for synthesizing 2D films often involve high-temperature synthesis, precursors, and growth stimulants with highly chemical reactivity. This limitation hinders the widespread applications of 2D films. As a result, reports concerning transfer strategies of 2D films from bare substrates to target substrates have proliferated, showcasing varying degrees of cleanliness, surface damage, and material uniformity. This review aims to evaluate, discuss, and provide an overview of the most advanced transfer methods to date, encompassing wet, dry, and quasi-dry transfer methods. The processes, mechanisms, and pros and cons of each transfer method are critically summarized. Furthermore, we discuss the feasibility of these 2D film transfer methods, concerning their applications in devices and various technology platforms.

Absorption of photons in atomically thin materials has become a challenge in the realization of ultrathin, high-performance optoelectronics. While numerous schemes have been used to enhance absorption in 2D semiconductors, such enhanced device performance in scalable monolayer photodetectors remains unattained. Here, we demonstrate wafer-scale integration of monolayer single-crystal MoS 2 photodetectors with a nitride-based resonant plasmonic metasurface to achieve a high detectivity of 2.58 × 10 12 Jones with a record-low dark current of 8 pA and long-term stability over 40 days. Upon comparison with control devices, we observe an overall enhancement factor of >100; this can be attributed to the local strong EM field enhanced photogating effect by the resonant plasmonic metasurface. Considering the compatibility of 2D semiconductors and hafnium nitride with the Si CMOS process and their scalability across wafer sizes, our results facilitate the smooth incorporation of 2D semiconductor-based photodetectors into the fields of imaging, sensing, and optical communication applications.

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) represent the ultimate thickness for scaling down channel materials. They provide a tantalizing solution to push the limit of semiconductor technology nodes in the sub-1 nm range. One key challenge with 2D semiconducting TMD channel materials is to achieve large-scale batch growth on insulating substrates of single crystals with spatial homogeneity and compelling electrical properties. Recent studies have claimed the epitaxy growth of wafer-scale, single-crystal 2D TMDs on a c-plane sapphire substrate with deliberately engineered off-cut angles. It has been postulated that exposed step edges break the energy degeneracy of nucleation and thus drive the seamless stitching of mono-oriented flakes. Here we show that a more dominant factor should be considered: in particular, the interaction of 2D TMD grains with the exposed oxygen-aluminium atomic plane establishes an energy-minimized 2D TMD-sapphire configuration. Reconstructing the surfaces of c-plane sapphire substrates to only a single type of atomic plane (plane symmetry) already guarantees the single-crystal epitaxy of monolayer TMDs without the aid of step edges. Electrical results evidence the structural uniformity of the monolayers. Our findings elucidate a long-standing question that curbs the wafer-scale batch epitaxy of 2D TMD single crystals-an important step towards using 2D materials for future electronics. Experiments extended to perovskite materials also support the argument that the interaction with sapphire atomic surfaces is more dominant than step-edge docking., (© 2023. The Author(s), under exclusive licence to Springer Nature Limited.)

Three-dimensional monolithic integration of memory devices with logic transistors is a frontier challenge in computer hardware. This integration is essential for augmenting computational power concurrent with enhanced energy efficiency in big data applications such as artificial intelligence. Despite decades of efforts, there remains an urgent need for reliable, compact, fast, energy-efficient and scalable memory devices. Ferroelectric field-effect transistors (FE-FETs) are a promising candidate, but requisite scalability and performance in a back-end-of-line process have proven challenging. Here we present back-end-of-line-compatible FE-FETs using two-dimensional MoS 2 channels and AlScN ferroelectric materials, all grown via wafer-scalable processes. A large array of FE-FETs with memory windows larger than 7.8 V, ON/OFF ratios greater than 10 7 and ON-current density greater than 250 μA um -1 , all at ~80 nm channel length are demonstrated. The FE-FETs show stable retention up to 10 years by extension, and endurance greater than 10 4  cycles in addition to 4-bit pulse-programmable memory features, thereby opening a path towards the three-dimensional heterointegration of a two-dimensional semiconductor memory with silicon complementary metal-oxide-semiconductor logic., (© 2023. The Author(s), under exclusive licence to Springer Nature Limited.)

Growing continuous monolayer films of transition-metal dichalcogenides (TMDs) without the disruption of grain boundaries is essential to realize the full potential of these materials for future electronics and optoelectronics, but it remains a formidable challenge. It is generally believed that controlling the TMDs orientations on epitaxial substrates stems from matching the atomic registry, symmetry, and penetrable van der Waals forces. Interfacial reconstruction within the exceedingly narrow substrate-epilayer gap has been anticipated. However, its role in the growth mechanism has not been intensively investigated. Here, we report the experimental conformation of an interfacial reconstructed (IR) layer within the substrate-epilayer gap. Such an IR layer profoundly impacts the orientations of nucleating TMDs domains and, thus, affects the materials' properties. These findings provide deeper insights into the buried interface that could have profound implications for the development of TMD-based electronics and optoelectronics.

Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in-plane ferroelectric material that exhibits a giant nonlinear optical effect, group-IV monochalcogenide SnSe, is reported. Nanometer-scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical-vapor-deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second-harmonic fields and the as-resulted second-harmonic generation was observed to be 100 times more intense than monolayer WS 2 . This work demonstrates in-plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on-chip nonlinear optical components and nonvolatile memory devices., (© 2023 Wiley-VCH GmbH.)

Tailoring of the propagation dynamics of exciton-polaritons in two-dimensional quantum materials has shown extraordinary promise to enable nanoscale control of electromagnetic fields. Varying permittivities along crystal directions within layers of material systems, can lead to an in-plane anisotropic dispersion of polaritons. Exploiting this physics as a control strategy for manipulating the directional propagation of the polaritons is desired and remains elusive. Here we explore the in-plane anisotropic exciton-polariton propagation in SnSe, a group-IV monochalcogenide semiconductor that forms ferroelectric domains and shows room-temperature excitonic behaviour. Exciton-polaritons are launched in SnSe multilayer plates, and their propagation dynamics and dispersion are studied. This propagation of exciton-polaritons allows for nanoscale imaging of the in-plane ferroelectric domains. Finally, we demonstrate the electric switching of the exciton-polaritons in the ferroelectric domains of this complex van der Waals system. The study suggests that systems such as group-IV monochalcogenides could serve as excellent ferroic platforms for actively reconfigurable polaritonic optical devices., (© 2023. The Author(s), under exclusive licence to Springer Nature Limited.)

Thin-film electronics pliably laminated onto the epidermis for noninvasive, specific, and multifunctional sensing are ideal wearable systems for health monitoring and information technologies. However, it remains a critical challenge to fabricate ultrathin and compliant skin-like sensors with high imperceptibility and sensitivities. Here we report a design of conductive hydrogen-substituted graphdiyne (HsGDY) nanofilms with conjugated porous structure and inherent softness for on-skin sensors that allow minimization of stress and discomfort with wear. Dominated by the subtle deformation-induced changes in the interdomain tunneling conductance, the engineered HsGDY sensors show continuous and accurate results. Real-time noninvasive spatial mapping of dynamic/static strains in both tensile/compressive directions monitors various body motions with high sensitivity (GF ∼22.6, under 2% strain), fast response (∼60 ms), and long-term durability (∼5000 cycles). Moreover, such devices can dynamically distinguish between the temperature difference and frequency of air inhaled and exhaled through the nostril, revealing a quantitative assessment of the movement/health of the human body. The proof-of-concept strategy provides an alternative route for the design of next-generation wearable organic bioelectronics with multiple electronic functionalities.

Architected materials that actively respond to external stimuli hold tantalizing prospects for applications in energy storage, wearable electronics, and bioengineering. Molybdenum disulfide, an excellent two-dimensional building block, is a promising candidate for lithium-ion battery anode. However, the stacked and brittle two-dimensional layered structure limits its rate capability and electrochemical stability. Here we report the dewetting-induced manufacturing of two-dimensional molybdenum disulfide nanosheets into a three-dimensional foam with a structural hierarchy across seven orders of magnitude. Our molybdenum disulfide foam provides an interpenetrating network for efficient charge transport, rapid ion diffusion, and mechanically resilient and chemically stable support for electrochemical reactions. These features induce a pseudocapacitive energy storage mechanism involving molybdenum redox reactions, confirmed by in-situ X-ray absorption near edge structure. The extraordinary electrochemical performance of molybdenum disulfide foam outperforms most reported molybdenum disulfide-based Lithium-ion battery anodes and state-of-the-art materials. This work opens promising inroads for various applications where special properties arise from hierarchical architecture., (© 2022. The Author(s).)

Solvent-solvent and solvent-anion pairings in battery electrolytes have been identified for the first time by nuclear magnetic resonance spectroscopy. These hitherto unknown interactions are enabled by the hydrogen bonding induced by the strong Lewis acid Li + , and exist between the electron-deficient hydrogen (δ + H) present in the solvent molecules and either other solvent molecules or negatively-charged anions. Complementary with the well-established strong but short-ranged Coulombic interactions between cation and solvent molecules, such weaker but longer-ranged hydrogen-bonding casts the formation of an extended liquid structure in electrolytes that is influenced by their components (solvents, additives, salts, and concentration), which in turn dictates the ion transport within bulk electrolytes and across the electrolyte-electrode interfaces. The discovery of this new inter-component force completes the picture of how electrolyte components interact and arrange themselves, sets the foundation to design better electrolytes on the fundamental level, and probes battery performances., (© 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.)

The development of membranes that block solutes while allowing rapid water transport is of great importance. The microstructure of the membrane needs to be rationally designed at the molecular level to achieve precise molecular sieving and high water flux simultaneously. We report the design and fabrication of ultrathin, ordered conjugated-polymer-framework (CPF) films with thicknesses down to 1 nm via chemical vapour deposition and their performance as separation membranes. Our CPF membranes inherently have regular rhombic sub-nanometre (10.3 × 3.7 Å) channels, unlike membranes made of carbon nanotubes or graphene, whose separation performance depends on the alignment or stacking of materials. The optimized membrane exhibited a high water/NaCl selectivity of ∼6,900 and water permeance of ∼112 mol m -2  h -1  bar -1 , and salt rejection >99.5% in high-salinity mixed-ion separations driven by osmotic pressure. Molecular dynamics simulations revealed that water molecules quickly and collectively pass through the membrane by forming a continuous three-dimensional network within the hydrophobic channels. The advent of ordered CPF provides a route towards developing carbon-based membranes for precise molecular separation., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

2D transition metal dichalcogenides (TMDCs) with intense and tunable photoluminescence (PL) have opened up new opportunities for optoelectronic and photonic applications such as light-emitting diodes, photodetectors, and single-photon emitters. Among the standard characterization tools for 2D materials, Raman spectroscopy stands out as a fast and non-destructive technique capable of probing material's crystallinity and perturbations such as doping and strain. However, a comprehensive understanding of the correlation between photoluminescence and Raman spectra in monolayer MoS 2 remains elusive due to its highly nonlinear nature. Here, the connections between PL signatures and Raman modes are systematically explored, providing comprehensive insights into the physical mechanisms correlating PL and Raman features. This study's analysis further disentangles the strain and doping contributions from the Raman spectra through machine-learning models. First, a dense convolutional network (DenseNet) to predict PL maps by spatial Raman maps is deployed. Moreover, a gradient boosted trees model (XGBoost) with Shapley additive explanation (SHAP) to bridge the impact of individual Raman features in PL features is applied. Last, a support vector machine (SVM) to project PL features on Raman frequencies is adopted. This work may serve as a methodology for applying machine learning to characterizations of 2D materials., (© 2022 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Two-dimensional (2D) semiconducting monolayers such as transition metal dichalcogenides (TMDs) are promising channel materials to extend Moore's Law in advanced electronics. Synthetic TMD layers from chemical vapor deposition (CVD) are scalable for fabrication but notorious for their high defect densities. Therefore, innovative endeavors on growth reaction to enhance their quality are urgently needed. Here, we report that the hydroxide W species, an extremely pure vapor phase metal precursor form, is very efficient for sulfurization, leading to about one order of magnitude lower defect density compared to those from conventional CVD methods. The field-effect transistor (FET) devices based on the proposed growth reach a peak electron mobility ~200 cm 2 /Vs (~800 cm 2 /Vs) at room temperature (15 K), comparable to those from exfoliated flakes. The FET device with a channel length of 100 nm displays a high on-state current of ~400 µA/µm, encouraging the industrialization of 2D materials., (© 2022. The Author(s).)

The scaling of silicon metal-oxide-semiconductor field-effect transistors has followed Moore's law for decades, but the physical thinning of silicon at sub-ten-nanometre technology nodes introduces issues such as leakage currents 1 . Two-dimensional (2D) layered semiconductors, with an atomic thickness that allows superior gate-field penetration, are of interest as channel materials for future transistors 2,3 . However, the integration of high-dielectric-constant (κ) materials with 2D materials, while scaling their capacitance equivalent thickness (CET), has proved challenging. Here we explore transferrable ultrahigh-κ single-crystalline perovskite strontium-titanium-oxide membranes as a gate dielectric for 2D field-effect transistors. Our perovskite membranes exhibit a desirable sub-one-nanometre CET with a low leakage current (less than 10 -2  amperes per square centimetre at 2.5 megavolts per centimetre). We find that the van der Waals gap between strontium-titanium-oxide dielectrics and 2D semiconductors mitigates the unfavourable fringing-induced barrier-lowering effect resulting from the use of ultrahigh-κ dielectrics 4 . Typical short-channel transistors made of scalable molybdenum-disulfide films by chemical vapour deposition and strontium-titanium-oxide dielectrics exhibit steep subthreshold swings down to about 70 millivolts per decade and on/off current ratios up to 10 7 , which matches the low-power specifications suggested by the latest International Roadmap for Devices and Systems 5 ., (© 2022. The Author(s), under exclusive licence to Springer Nature Limited.)

Design and development of an efficient, nonprecious catalyst with structural features and functionality necessary for driving the hydrogen evolution reaction (HER) in an alkaline medium remain a formidable challenge. At the root of the functional limitation is the inability to tune the active catalytic sites while overcoming the poor reaction kinetics observed under basic conditions. Herein, we report a facile approach to enable the selective design of an electrochemically efficient cobalt phosphide oxide composite catalyst on carbon cloth (CoP-Co x O y /CC), with good activity and durability toward HER in alkaline medium (η 10 = -43 mV). Theoretical studies revealed that the redistribution of electrons at laterally dispersed Co phosphide/oxide interfaces gives rise to a synergistic effect in the heterostructured composite, by which various Co oxide phases initiate the dissociation of the alkaline water molecule. Meanwhile, the highly active CoP further facilitates the adsorption-desorption process of water electrolysis, leading to extremely high HER activity.

Two-dimensional (2D) transition metal dichalcogenide (TMDC) monolayers have been widely used for optoelectronic devices because of their ultrasensitivity to light detection acquired from their direct gap properties. However, the small cross-section of photon absorption in the atomically thin layer thickness significantly limits the generation of photocarriers, restricting their performance. Here, we integrate monolayer WS 2 with 2D perovskites Cs 2 AgBiBr 6 , which serve as the light absorption layer, to greatly enhance the photosensitivity of WS 2 . The efficient charge transfer at the Cs 2 AgBiBr 6 /WS 2 heterojunction is evidenced by the shortened photoluminescence (PL) decay time of Cs 2 AgBiBr 6 . Scanning photocurrent microscopy of Cs 2 AgBiBr 6 /WS 2 /graphene reveals that improved charge extraction from graphene leads to an enhanced photoresponse. The 2D Cs 2 AgBiBr 6 /WS 2 /graphene vertical heterostructure photodetector exhibits a high detectivity ( D *) of 1.5 × 10 13 Jones with a fast response time of 52.3 μs/53.6 μs and an on/off ratio of 1.02 × 10 4 . It is worth noting that this 2D heterostructure photodetector can realize self-powered light detection behavior with an open-circuit voltage of ∼0.75 V. The results suggest that the 2D perovskites can effectively improve the TMDC layer-based photodetectors for low-power consumption photoelectrical applications.

A facile solvothermal synthesis approach for chemical composition control in ternary Bi-S-I systems is reported by simply controlling the sulfide concentration. We demonstrate the application of these bismuth-based ternary mixed-anion compounds as high capacity anode materials in rechargeable batteries. Cells utilising Bi 13 S 18 I 2 achieved an initial capacity value of 807 mA h g -1 , while those with BiSI/Bi 13 S 18 I 2 a value of 1087 mA h g -1 in lithium-ion battery systems.

Two-dimensional (2D) layered materials hold tremendous promise for post-Si nanoelectronics due to their unique optical and electrical properties. Significant advances have been achieved in device fabrication and synthesis routes for 2D nanoelectronics over the past decade; however, one major bottleneck preventing their immediate applications has been the lack of a reproducible approach for growing wafer-scale single-crystal films despite tremendous progress in recent experimental demonstrations. In this tutorial review, we provide a systematic summary of the critical factors-including crystal/substrate symmetry and energy consideration-necessary for synthesizing single-orientation 2D layers. In particular, we focus on the discussions of the atomic edge-guided epitaxial growth, which assists in unidirectional nucleation for the wafer-scale growth of single-crystal 2D layers.

A comprehensive understanding of the energy level alignment mechanisms between two-dimensional (2D) semiconductors and electrodes is currently lacking, but it is a prerequisite for tailoring the interface electronic properties to the requirements of device applications. Here, we use angle-resolved direct and inverse photoelectron spectroscopy to unravel the key factors that determine the level alignment at interfaces between a monolayer of the prototypical 2D semiconductor MoS 2 and conductor, semiconductor, and insulator substrates. For substrate work function (Φ sub ) values below 4.5 eV we find that Fermi level pinning occurs, involving electron transfer to native MoS 2 gap states below the conduction band. For Φ sub above 4.5 eV, vacuum level alignment prevails but the charge injection barriers do not strictly follow the changes of Φ sub as expected from the Schottky-Mott rule. Notably, even the trends of the injection barriers for holes and electrons are different. This is caused by the band gap renormalization of monolayer MoS 2 by dielectric screening, which depends on the dielectric constant (ε r ) of the substrate. Based on these observations, we introduce an expanded Schottky-Mott rule that accounts for band gap renormalization by ε r -dependent screening and show that it can accurately predict charge injection barriers for monolayer MoS 2 . It is proposed that the formalism of the expanded Schottky-Mott rule should be universally applicable for 2D semiconductors, provided that material-specific experimental benchmark data are available.

Electronic charge rearrangement between components of a heterostructure is the fundamental principle to reach the electronic ground state. It is acknowledged that the density of state distribution of the components governs the amount of charge transfer, but a notable dependence on temperature is not yet considered, particularly for weakly interacting systems. Here, it is experimentally observed that the amount of ground-state charge transfer in a van der Waals heterostructure formed by monolayer MoS 2 sandwiched between graphite and a molecular electron acceptor layer increases by a factor of 3 when going from 7 K to room temperature. State-of-the-art electronic structure calculations of the full heterostructure that accounts for nuclear thermal fluctuations reveal intracomponent electron-phonon coupling and intercomponent electronic coupling as the key factors determining the amount of charge transfer. This conclusion is rationalized by a model applicable to multicomponent van der Waals heterostructures., (© 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

Conjugated polyaniline can impact the field of water filtration membranes due to its hydrophilic and antibacterial nature, facile and inexpensive synthesis procedure, heat and acid tolerance, and unique doping/dedoping chemistry. However, the gelation effect, its rigid backbone, and the limited hydrophilicity of polyaniline severely restrict the adaptability to membranes and their antifouling performance. This Mini Review summarizes important works of polyaniline-related ultrafiltration membranes, highlighting solutions to conquer engineering obstacles in processing and challenges in enhancing surface hydrophilicity with an emphasis on chemistry. As a pH-responsive polymer convertible to a conductive salt, this classic material should continue to bring unconventional advances into the realm of water filtration membranes.

Van der Waals heterostructures consisting of 2D semiconductors and conjugated molecules are of increasing interest because of the prospect of a synergistic enhancement of (opto)electronic properties. In particular, perylenetetracarboxylic dianhydride (PTCDA) on monolayer (ML)-MoS 2 has been identified as promising candidate and a staggered type-II energy level alignment and excited state interfacial charge transfer have been proposed. In contrast, it is here found with inverse and direct angle resolved photoelectron spectroscopy that PTCDA/ML-MoS 2 supported by insulating sapphire exhibits a straddling type-I level alignment, with PTCDA having the wider energy gap. Photoluminescence (PL) and sub-picosecond transient absorption measurements reveal that resonance energy transfer, i.e., electron-hole pair (exciton) transfer, from PTCDA to ML-MoS 2 occurs on a sub-picosecond time scale. This gives rise to an enhanced PL yield from ML-MoS 2 in the heterostructure and an according overall modulation of the photoresponse. These results underpin the importance of a precise knowledge of the interfacial electronic structure in order to understand excited state dynamics and to devise reliable design strategies for optimized optoelectronic functionality in van der Waals heterostructures., Competing Interests: The authors declare no conflict of interest., (© 2021 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

The photoelectrochemical (PEC) approach is attractive as a promising route for the nitrogen reduction reaction (NRR) toward ammonia (NH 3 ) synthesis. However, the challenges in synergistic management of optical, electrical, and catalytic properties have limited the efficiency of PEC NRR devices. Herein, to enhance light-harvesting, carrier separation/transport, and the catalytic reactions, a concept of decoupling light-harvesting and electrocatalysis by employing a cascade n + np + -Si photocathode is implemented. Such a decoupling design not only abolishes the parasitic light blocking but also concurrently improves the optical and electrical properties of the n + np + -Si photocathode without compromising the efficiency. Experimental and density functional theory studies reveal that the porous architecture and N-vacancies promote N 2 adsorption of the Au/porous carbon nitride (PCN) catalyst. Impressively, an n + np + -Si photocathode integrating the Au/PCN catalyst exhibits an outstanding PEC NRR performance with maximum Faradaic efficiency (FE) of 61.8% and NH 3 production yield of 13.8 µg h -1 cm -2 at -0.10 V versus reversible hydrogen electrode (RHE), which is the highest FE at low applied potential ever reported for the PEC NRR., (© 2021 Wiley-VCH GmbH.)

Advanced beyond-silicon electronic technology requires both channel materials and also ultralow-resistance contacts to be discovered 1,2 . Atomically thin two-dimensional semiconductors have great potential for realizing high-performance electronic devices 1,3 . However, owing to metal-induced gap states (MIGS) 4-7 , energy barriers at the metal-semiconductor interface-which fundamentally lead to high contact resistance and poor current-delivery capability-have constrained the improvement of two-dimensional semiconductor transistors so far 2,8,9 . Here we report ohmic contact between semimetallic bismuth and semiconducting monolayer transition metal dichalcogenides (TMDs) where the MIGS are sufficiently suppressed and degenerate states in the TMD are spontaneously formed in contact with bismuth. Through this approach, we achieve zero Schottky barrier height, a contact resistance of 123 ohm micrometres and an on-state current density of 1,135 microamps per micrometre on monolayer MoS 2 ; these two values are, to the best of our knowledge, the lowest and highest yet recorded, respectively. We also demonstrate that excellent ohmic contacts can be formed on various monolayer semiconductors, including MoS 2 , WS 2 and WSe 2 . Our reported contact resistances are a substantial improvement for two-dimensional semiconductors, and approach the quantum limit. This technology unveils the potential of high-performance monolayer transistors that are on par with state-of-the-art three-dimensional semiconductors, enabling further device downscaling and extending Moore's law.

Two-dimensional transition metal dichalcogenide nanoribbons are touted as the future extreme device downscaling for advanced logic and memory devices but remain a formidable synthetic challenge. Here, we demonstrate a ledge-directed epitaxy (LDE) of dense arrays of continuous, self-aligned, monolayer and single-crystalline MoS 2 nanoribbons on β-gallium (III) oxide (β-Ga 2 O 3 ) (100) substrates. LDE MoS 2 nanoribbons have spatial uniformity over a long range and transport characteristics on par with those seen in exfoliated benchmarks. Prototype MoS 2 -nanoribbon-based field-effect transistors exhibit high on/off ratios of 10 8 and an averaged room temperature electron mobility of 65 cm 2  V -1  s -1 . The MoS 2 nanoribbons can be readily transferred to arbitrary substrates while the underlying β-Ga 2 O 3 can be reused after mechanical exfoliation. We further demonstrate LDE as a versatile epitaxy platform for the growth of p-type WSe 2 nanoribbons and lateral heterostructures made of p-WSe 2 and n-MoS 2 nanoribbons for futuristic electronics applications.

Skin-mountable microelectronics are garnering substantial interest for various promising applications including human-machine interfaces, biointegrated devices, and personalized medicine. However, it remains a critical challenge to develop e-skins to mimic the human somatosensory system in full working range. Here, we present a multifunctional e-skin system with a heterostructured configuration that couples vinyl-hybrid-silica nanoparticle (VSNP)-modified polyacrylamide (PAM) hydrogel with two-dimensional (2D) MXene through nano-bridging layers of polypyrrole nanowires (PpyNWs) at the interfaces, featuring high toughness and low hysteresis, in tandem with controlled crack generation and distribution. The multidimensional configurations endow the e-skin with an extraordinary working range (2800%), ultrafast responsiveness (90 ms) and resilience (240 ms), good linearity (800%), tunable sensing mechanisms, and excellent reproducibility. In parallel, this e-skin platform is capable of detecting, quantifying, and remotely monitoring stretching motions in multiple dimensions, tactile pressure, proximity sensing, and variations in temperature and light, establishing a promising platform for next-generation smart flexible electronics., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).)

High-resolution scanning transmission electron microscopy (HR-STEM) with spherical aberration correction enables researchers to peer into two-dimensional (2D) materials and correlate the material properties with those of single atoms. The maximum intensity of corrected electron beam is confined in the area having sub-angstrom size. Meanwhile, the residual threefold astigmatism of the electron probe implies a triangular shape distribution of the intensity, whereas its tails overlap and thus interact with several atomic species simultaneously. The result is the resonant modulation of contrast that interferes the determination of phase transition of 2D materials. Here, we theoretically reveal and experimentally determine the origin of resonant modulation of contrast and its unintended impact on violating the power-law dependence of contrast on coordination modes between transition metal and chalcogenide atoms. The finding illuminates the correlation between atomic contrast, spatially inequivalent chalcogenide orientation, and residual threefold astigmatism on determining the atomic structure of emerging 2D materials., (Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).)

The optoelectronic properties of atomically thin transition-metal dichalcogenides are strongly correlated with the presence of defects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge generation and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS 2 monolayers by laser-illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals, respectively. Time-resolved experiments indicate that the critical process for photoexcited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the long-lived photoconductivity signal is higher in chemical-vapor deposited (CVD) samples than exfoliated monolayers due to the presence of traps that inhibits recombination. Our work reveals the intrinsic time and length scales of electrical response to photoexcitation in van der Waals materials, which is essential for their applications in optoelectronic devices., Competing Interests: The authors declare no competing interest.

The application of liquid-exfoliated 2D transition metal disulfides (TMDs) as the hole transport layers (HTLs) in nonfullerene-based organic solar cells is reported. It is shown that solution processing of few-layer WS 2 or MoS 2 suspensions directly onto transparent indium tin oxide (ITO) electrodes changes their work function without the need for any further treatment. HTLs comprising WS 2 are found to exhibit higher uniformity on ITO than those of MoS 2 and consistently yield solar cells with superior power conversion efficiency (PCE), improved fill factor (FF), enhanced short-circuit current (J SC ), and lower series resistance than devices based on poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) and MoS 2 . Cells based on the ternary bulk-heterojunction PBDB-T-2F:Y6:PC 71 BM with WS 2 as the HTL exhibit the highest PCE of 17%, with an FF of 78%, open-circuit voltage of 0.84 V, and a J SC of 26 mA cm -2 . Analysis of the cells' optical and carrier recombination characteristics indicates that the enhanced performance is most likely attributed to a combination of favorable photonic structure and reduced bimolecular recombination losses in WS 2 -based cells. The achieved PCE is the highest reported to date for organic solar cells comprised of 2D charge transport interlayers and highlights the potential of TMDs as inexpensive HTLs for high-efficiency organic photovoltaics., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Wearable and portable self-powered units have stimulated considerable attention in both the scientific and technological realms. However, their innovative development is still limited by inefficient bulky connections between functional modules, incompatible energy storage systems with poor cycling stability, and real safety concerns. Herein, we demonstrate a flexible solar-charging integrated unit based on the design of printed magnesium ion aqueous asymmetric supercapacitors. This power unit exhibits excellent mechanical robustness, high photo-charging cycling stability (98.7% capacitance retention after 100 cycles), excellent overall energy conversion and storage efficiency (η overall  = 17.57%), and outstanding input current tolerance. In addition, the Mg ion quasi-solid-state asymmetric supercapacitors show high energy density up to 13.1 mWh cm -3 via pseudocapacitive ion storage as investigated by an operando X-ray diffraction technique. The findings pave a practical route toward the design of future self-powered systems affording favorable safety, long life, and high energy.

Memristive devices have been extensively demonstrated for applications in nonvolatile memory, computer logic, and biological synapses. Precise control of the conducting paths associated with the resistance switching in memristive devices is critical for optimizing their performances including ON/OFF ratios. Here, gate tunability and multidirectional switching can be implemented in memristors for modulating the conducting paths using hexagonal α-In 2 Se 3 , a semiconducting van der Waals ferroelectric material. The planar memristor based on in-plane (IP) polarization of α-In 2 Se 3 exhibits a pronounced switchable photocurrent, as well as gate tunability of the channel conductance, ferroelectric polarization, and resistance-switching ratio. The integration of vertical α-In 2 Se 3 memristors based on out-of-plane (OOP) polarization is demonstrated with a device density of 7.1 × 10 9 in. -2 and a resistance-switching ratio of well over 10 3 . A multidirectionally operated α-In 2 Se 3 memristor is also proposed, enabling the control of the OOP (or IP) resistance state directly by an IP (or OOP) programming pulse, which has not been achieved in other reported memristors. The remarkable behavior and diverse functionalities of these ferroelectric α-In 2 Se 3 memristors suggest opportunities for future logic circuits and complex neuromorphic computing., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The facile synthesis of hierarchically functional, catalytically active, and electrochemically stable nanostructures holds a tremendous promise for catalyzing the efficient and durable oxygen evolution reaction (OER) and yet remains a formidable challenge. Herein, we report the scalable production of core-shell nanostructures composed of carbon-coated cobalt diphosphide nanosheets, C@CoP 2 , via three simple steps: (i) electrochemical deposition of Co species, (ii) gas-phase phosphidation, and (iii) carbonization of CoP 2 for catalytic durability enhancement. Electrochemical characterizations showed that C@CoP 2 delivers an overpotential of 234 mV, retains its initial activity for over 80 h of continuous operation, and exhibits a fast OER rate of 63.8 mV dec -1 in base.

2D transition metal dichalcogenide (TMD) layered materials are promising for future electronic and optoelectronic applications. The realization of large-area electronics and circuits strongly relies on wafer-scale, selective growth of quality 2D TMDs. Here, a scalable method, namely, metal-guided selective growth (MGSG), is reported. The success of control over the transition-metal-precursor vapor pressure, the first concurrent growth of two dissimilar monolayer TMDs, is demonstrated in conjunction with lateral or vertical TMD heterojunctions at precisely desired locations over the entire wafer in a single chemical vapor deposition (VCD) process. Owing to the location selectivity, MGSG allows the growth of p- and n-type TMDs with spatial homogeneity and uniform electrical performance for circuit applications. As a demonstration, the first bottom-up complementary metal-oxide-semiconductor inverter based on p-type WSe 2 and n-type MoSe 2 is achieved, which exhibits a high and reproducible voltage gain of 23 with little dependence on position., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The highly prevalent and virulent disease in the Western Hemisphere Coccidioidomycosis, also known as Valley Fever, can cause serious illness such as severe pneumonia with respiratory failure. It can also take on a disseminated form where the infection spreads throughout the body. Thus, a serious impetus exists to develop effective detection of the disease that can also operate in a rapid and high-throughput fashion. Here, we report the assembly of a highly sensitive biosensor using reduced graphene oxide (rGO) with Coccidioides(cocci) antibodies as the target analytes. The facile design made possible by the scalable microcontact printing (μCP) surface patterning technique which enables rapid, ultrasensitive detection. It provides a wide linear range and sub picomolar (2.5 pg/ml) detection, while also delivering high selectivity and reproducibility. This work demonstrates an important advancement in the development of a sensitive label-free rGO biosensor for Coccidioidomycosis detection. This result also provides the potential application of direct pathogen diagnosis for the future biosensor development., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Surface functionalization of nanoscale materials has a significant impact on their properties. We have demonstrated the effect of different passivating ligands on the crystal phase of organometal halide perovskite quantum dots (PQDs). Using static and dynamic spectroscopy, we studied phase transitions in CH 3 NH 3 PbBr 3 PQDs ligated with either octylaminebromide (P-OABr) or 3-aminopropyl triethoxysilane (P-APTES). Around 140 K, P-OABr underwent a structural phase transition from tetragonal to orthorhombic, established by the emergence of a higher energy band in the photoluminescence (PL) spectrum. This was not observed in P-APTES, despite cooling down to 20 K. Additionally, time-resolved and excitation power-dependent PL, as well as Raman spectroscopy over a range of 300-20 K, revealed that recombination rates and types of charge carriers involved are significantly different in P-APTES and P-OABr. Our findings highlight how aspects of PQD phase stabilization are linked to nanoscale morphology and the crystal phase diagram.

The emerging molybdenum disulfide (MoS 2 ) offers intriguing possibilities for realizing a transformative new catalyst for driving the hydrogen evolution reaction (HER). However, the trade-off between catalytic activity and long-term stability represents a formidable challenge and has not been extensively addressed. This study reports that metastable and temperature-sensitive chemically exfoliated MoS 2 (ce-MoS 2 ) can be made into electrochemically stable (5000 cycles), and thermally robust (300 °C) while maintaining synthetic scalability and excellent catalytic activity through physical-transformation into 3D structurally deformed nanostructures. The dimensional transition enabled by a high throughput electrohydrodynamic process provides highly accessible, and electrochemically active surface area and facilitates efficient transport across various interfaces. Meanwhile, the hierarchically strained morphology is found to improve electronic coupling between active sites and current collecting substrates without the need for selective engineering the electronically heterogeneous interfaces. Specifically, the synergistic combination of high strain load stemmed from capillarity-induced-self-crumpling and sulfur (S) vacancies intrinsic to chemical exfoliation enables simultaneous modulation of active site density and intrinsic HER activity regardless of continuous operation or elevated temperature. These results provide new insights into how catalytic activity, electrochemical-, and thermal stability can be concurrently enhanced through the physical transformation that is reminiscent of nature, in which properties of biological materials emerge from evolved dimensional transitions., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The tantalizing prospect of harnessing the unique properties of graphene crumpled nanostructures continues to fuel tremendous interest in energy storage and harvesting applications. However, the paper ball-like, hard texture, and closed-sphere morphology of current 3D graphitic nanostructure production not only constricts the conductive pathways but also limits the accessible surface area. Here, we report new insights into electrohydrodynamically-generated droplets as colloidal nanoreactors in that the stimuli-responsive nature of reduced graphene oxide can lead to the formation of crumpled nanostructures with a combination of open structures and doubly curved, saddle-shaped edges. In particular, the crumpled nanostructures dynamically adapt to non-spherical, polyhedral shapes under continuous deposition, ultimately assembling into foam-like microstructures with a highly accessible surface area and spatially interconnected transport pathways. The implementation of such crumpled nanostructures as three-dimensional rear contacts for solar conversion applications realize benefits of a high aspect ratio, electrically addressable and energetically favorable interfaces, and substantial enhancement of both short-circuit currents and fill-factors compared to those made of planar graphene counterparts. Further, the 3D crumpled nanostructures may shed lights onto the development of effective electrocatalytic electrodes due to their open structure that simultaneously allows for efficient water flow and hydrogen escape.

We recorded gestational weight gain (GWG) and change in body mass index (BMI) at 28 weeks gestation in 343 vs. 339 women with and without gestational diabetes (GDM). GDM was associated with a greater increment in BMI, but not with increased GWG in kilograms., (Crown Copyright © 2014. Published by Elsevier Ireland Ltd. All rights reserved.)

Background: The role of laparoscopy in the management of diverticular disease is evolving. Concerns were raised in the past because laparoscopic resection for diverticulitis is often difficult and occasionally hazardous. This study was undertaken to evaluate the difference in overall outcomes between elective open and laparoscopic surgery with or without anastomosis for diverticulitis., Methods: Using the National Inpatient Sample (NIS) database, clinical data of patients who underwent elective open and laparoscopic surgery (lap) for diverticulitis from 2002 to 2007 were collected and analyzed. Patients who underwent emergent surgery were excluded., Results: A total of 124,734 patients underwent elective surgery for diverticulitis: open, 110,172 (88.3%); lap, 14,562 (11.7%). The overall intraoperative complication rate was significantly lower in the laparoscopy group (0.63% vs. 1.15%, P < 0.01). However, there was no significant difference observed in ureteral injury between groups (open, 0.17%; lap, 0.12%, P = 0.15). All evaluated postoperative complications (ileus, abdominal abscess, leak, wound infection, bowel obstruction, urinary tract infection, pneumonia, respiratory failure, venous thromboembolism) were significantly higher for the open procedures. The laparoscopy group had a shorter mean hospital stay (lap, 5.06 days; open, 6.68 days, P < 0.01) and lower total hospital charges (lap, $36,389; open, $39,406, P < 0.01) than the open group. Also, mortality was four times higher in the open group (open, 0.54%; lap, 0.13%, P < 0.01)., Conclusions: The laparoscopic operation was associated with lower morbidity, lower mortality, shorter hospital stay, and lower hospital charges compared to the open operation for diverticulitis. Elective laparoscopic surgery for diverticulitis is safe and can be considered the preferred operative option.

Etoricoxib is an anti-inflammatory drug largely used in a variety of acute and chronic inflammatory diseases, but is associated with low aqueous solubility and poor dissolution leading to a delayed rate of absorption and onset of action. This study focuses on the development and pharmacological evaluation of a series of binary systems of etoricoxib with cyclodextrins. The binary systems of etoricoxib with beta-cyclodextrin (beta-CD) and 2-hydroxypropyl-beta-cyclodextrin (HP-beta-CD) were prepared by the kneading method. Drug-cyclodextrin interactions in solution were investigated by the phase solubility analysis. X-ray diffractometry studies were carried out for the characterization of all binary systems. In vivo studies were performed using the tail flick and Eddy's hot plate apparatus. The results of the phase solubility studies indicated an increase in etoricoxib solubility upon complexation with beta-cyclodextrin (stability constant, Kc value of 198.6 and 209.9 L/mol for 1:1 and 1:2 beta-CD complexes of the drug, respectively) and a further increase on complexation with HP-beta-CD (stability constant, Kc value of 265.3 and 355.8 L/mol for 1:1 and 1:2 HP-beta-CD complexes of the drug, respectively). Results of the in vivo drug activity studies also pointed towards an enhanced antinociceptive effect of etoricoxib upon cyclodextrin complexation with 1:2 drug HP-beta-CD complex showing maximum effect.

RNA splicing is an essential step in gene expression, and is often variable, giving rise to multiple alternatively spliced mRNA and protein isoforms from a single gene locus. The design of effective databases to support experimental and computational investigations of alternative splicing (AS) is a significant challenge. In an effort to integrate accurate exon and splice site annotation with current knowledge about splicing regulatory elements and predicted AS events, and to link information about the splicing of orthologous genes in different species, we have developed the Hollywood system. This database was built upon genomic annotation of splicing patterns of known genes derived from spliced alignment of complementary DNAs (cDNAs) and expressed sequence tags, and links features such as splice site sequence and strength, exonic splicing enhancers and silencers, conserved and non-conserved patterns of splicing, and cDNA library information for inferred alternative exons. Hollywood was implemented as a relational database and currently contains comprehensive information for human and mouse. It is accompanied by a web query tool that allows searches for sets of exons with specific splicing characteristics or splicing regulatory element composition, or gives a graphical or sequence-level summary of splicing patterns for a specific gene. A streamlined graphical representation of gene splicing patterns is provided, and these patterns can alternatively be layered onto existing information in the UCSC Genome Browser. The database is accessible at http://hollywood.mit.edu.

Exonic splicing silencers (ESSs) are cis-regulatory elements that inhibit the use of adjacent splice sites, often contributing to alternative splicing (AS). To systematically identify ESSs, an in vivo splicing reporter system was developed to screen a library of random decanucleotides. The screen yielded 141 ESS decamers, 133 of which were unique. The silencer activity of over a dozen of these sequences was also confirmed in a heterologous exon/intron context and in a second cell type. Of the unique ESS decamers, most could be clustered into groups to yield seven putative ESS motifs, some resembling known motifs bound by hnRNPs H and A1. Potential roles of ESSs in constitutive splicing were explored using an algorithm, ExonScan, which simulates splicing based on known or putative splicing-related motifs. ExonScan and related bioinformatic analyses suggest that these ESS motifs play important roles in suppression of pseudoexons, in splice site definition, and in AS.