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Implantable systems with chronic stability, high sensing performance, and extensive spatial-temporal resolution are a growing focus for monitoring and treating several diseases such as epilepsy, Parkinson's disease, chronic pain, and cardiac arrhythmias. These systems demand exceptional bendability, scalable size, durable electrode materials, and well-encapsulated metal interconnects. However, existing chronic implantable bioelectronic systems largely rely on materials prone to corrosion in biofluids, such as silicon nanomembranes or metals. This study introduces a multielectrode array featuring a wide bandgap (WBG) material as electrodes, demonstrating its suitability for chronic implantable applications. Our devices exhibit excellent flexibility and longevity, taking advantage of the low bending stiffness and chemical inertness in WBG nanomembranes and multimodalities for physical health monitoring, including temperature, strain, and impedance sensing. Our top-down manufacturing process enables the formation of distributed electrode arrays that can be seamlessly integrated onto the curvilinear surfaces of skins. As proof of concept for chronic cardiac pacing applications, we demonstrate the effective pacing functionality of our devices on rabbit hearts through a set of ex vivo experiments. The engineering approach proposed in this study overcomes the drawbacks of prior WBG material fabrication techniques, resulting in an implantable system with high bendability, effective pacing, and high-performance sensing.

The pursuit of increased efficiency of photoelectric energy conversion through optimized semiconductor structures remains highly competitive, with current results yet to align with broad expectations. In this study, we discover a significant enhancement in photocurrent performance of a p-3C-SiC nanothin film on p-Si/n-Si double junction (DJ) heterostructure that integrates p-3C-SiC/p-Si heterojunction and p-Si/n-Si homojunction. The vertical photocurrent (VPC) and vertical photoresponsivity exhibit a substantial enhancement in the DJ heterostructure, surpassing by a maximum of 43-fold compared to the p-3C-SiC/n-Si single junction (SJ) counterpart. The p-3C-SiC layer and n-Si substrate of the two heterostructures have similar material and geometrical properties. More importantly, the fabrication costs for the DJ and SJ heterostructure devices are comparable. Our results demonstrate a significant potential for using DJ devices in energy harvesters, micro/nano electromechanical systems, and sensing applications. This research may also lead to the creation of advanced optoelectronic devices using DJ structures, where employing various semiconductor materials to achieve exceptional performance through the application of the concept and theoretical model described in this work.

The development of fifth-generation (5G) communications and the Internet of Things (IoT) has created a need for high-performance sensing networks and sensors. Improving the sensitivity and reducing the energy consumption of these sensors can improve the performance of the sensing network and conserve energy. This paper reports a large enhancement of the photovoltaic effect in a 3C-SiC/Si heterostructure and the tunability of the photovoltage under the impact of a temperature gradient, which has the potential to increase the sensitivity and reduce the energy consumption of microsensors. To start with, cubic silicon carbide (3C-SiC) was grown on a silicon wafer, and a micro-3C-SiC/Si heterostructure device was then fabricated using standard photolithography. The result revealed that the sensor could either capture light energy, transform it into electrical energy for self-power purposes, or detect light with intensities of 1.6 and 4 mW/cm 2 . Under the impact of the temperature gradient induced by conduction heat transfer from a heater, the measured photovoltage was improved. This thermo-phototronic coupling enhanced the photovoltage up to 51% at a temperature gradient of 8.73 K and light intensity of 4 mW/cm 2 . Additionally, the enhancement can be tuned by controlling the direction of the temperature gradient and the temperature difference. These findings indicate the promise of the temperature gradient in SiC/Si heterostructures for developing high-performance temperature sensors and self-powered photodetectors.

Electrohydrodynamic atomization (EHDA) provides unparalleled control over the size and production rate of particles from solution. However, conventional methods produce highly charged particles that are not appropriate for inhalation drug delivery. We present a self-propelled EHDA system to address this challenge, a promising one-step platform for generating and delivering charge-reduced particles. Our approach uses a sharp electrode to produce ion wind, which reduces the cumulative charge in the particles and transports them to a target in front of the nozzle. We effectively controlled the morphologies of polymer products created from poly(vinylidene fluoride) (PVDF) at various concentrations. Our technique has also been proven safe for bioapplications, as evidenced by the delivery of PVDF particles onto breast cancer cells. The combination of simultaneous particle production and charge reduction, along with its direct delivery capability, makes the self-propelled EHDA a versatile technique for drug delivery applications.

The integration of micro- and nanoelectronics into or onto biomedical devices can facilitate advanced diagnostics and treatments of digestive disorders, cardiovascular diseases, and cancers. Recent developments in gastrointestinal endoscopy and balloon catheter technologies introduce promising paths for minimally invasive surgeries to treat these diseases. However, current therapeutic endoscopy systems fail to meet requirements in multifunctionality, biocompatibility, and safety, particularly when integrated with bioelectronic devices. Here, we report materials, device designs, and assembly schemes for transparent and stable cubic silicon carbide (3C-SiC)-based bioelectronic systems that facilitate tissue ablation, with the capability for integration onto the tips of endoscopes. The excellent optical transparency of SiC-on-glass (SoG) allows for direct observation of areas of interest, with superior electronic functionalities that enable multiple biological sensing and stimulation capabilities to assist in electrical-based ablation procedures. Experimental studies on phantom, vegetable, and animal tissues demonstrated relatively short treatment times and low electric field required for effective lesion removal using our SoG bioelectronic system. In vivo experiments on an animal model were conducted to explore the versatility of SoG electrodes for peripheral nerve stimulation, showing an exciting possibility for the therapy of neural disorders through electrical excitation. The multifunctional features of SoG integrated devices indicate their high potential for minimally invasive, cost-effective, and outcome-enhanced surgical tools, across a wide range of biomedical applications.

A metal-free scalable synthesis of functionalized ketenimines from alkyl α-(aryl/heteroaryl)-α-diazoacetates and alkyl isocyanides induced by blue light irradiation has been developed. The reaction proceeds at room temperature without any photocatalyst and provides ketenimines in moderate to good yields. Density functional theory (DFT) calculations and the experimental study showed that aryl(alkoxycarbonyl)carbenes in both singlet and triplet states can react with isocyanides but only the reaction of the former leads to the smooth formation of ketenimines. The obtained ketenimines were used for the synthesis of functionalized amidines under mild metal-free conditions., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

Giant piezoresistive effect enables the development of ultrasensitive sensing devices to address the increasing demands from hi-tech applications such as space exploration and self-driving cars. The discovery of the giant piezoresistive effect by optoelectronic coupling leads to a new strategy for enhancing the sensitivity of mechanical sensors, particularly with light from light-emitting diodes (LEDs). This paper reports on the piezoresistive effect in a 3C-SiC/Si heterostructure with a bonded LED that can reach a gauge factor (GF) as high as 18 000. This value represents an approximately 1000 times improvement compared to the configuration without a bonded LED. This GF is one of the highest GFs reported to date for the piezoresistive effect in semiconductors. The generation of carrier concentration gradient in the top thin 3C-SiC film under illumination from the LED coupling with the tuning current contributes to the modulation of the piezoresistive effect in a 3C-SiC/Si heterojunction. In addition, the feasibility of using different types of LEDs as the tools for modulating the piezoresistive effect is investigated by evaluating lateral photovoltage and photocurrent under LED's illumination. The generated lateral photovoltage and photocurrent are as high as 14 mV and 47.2 μA, respectively. Recent technologies for direct bonding of micro-LEDs on a Si-based device and the discovery reported here may have a significant impact on mechanical sensors.

Developing sensing approaches that can exploit visible light for the detection of low-concentration hydrogen at room temperatures has become increasingly important for the safe use of hydrogen in many applications. In this study, heterostructures composed of monolayer MoS 2 and Pd nanoclusters (Pd/MoS 2 ) acting as photo- and hydrogen-sensitizers are successfully fabricated in a facile and scalable manner. The uniform deposition of morphologically isotropic Pd nanoclusters (11.5 ± 2.2 nm) on monolayer MoS 2 produces a plethora of active heterojunctions, effectively suppressing charge carrier recombination under light illumination. The dual photo- and hydrogen-sensitizing functionality of Pd/MoS 2 can enable its use as an active sensing layer in optoelectronic hydrogen sensors. Gas-sensing examinations reveal that the sensing performance of Pd/MoS 2 is enhanced three-fold under visible light illumination (17% for 140 ppm of H 2 ) in comparison with dark light (5% for 140 ppm of H 2 ). Photoactivation is also found to enable excellent sensing reversibility and reproducibility in the obtained sensor. As a proof-of-concept, the integration of Pd nanoclusters and monolayer MoS 2 can open a new avenue for light-induced hydrogen gas sensing at room temperature.

Theoretically, the edges of a MoS 2 flake and S-vacancy within the lattice have nearly zero Gibbs free energy for hydrogen adsorption, which is essentially correlated to the exchange currents in hydrogen evolution reaction (HER). However, MoS 2 possesses insufficient active sites (edges and S-vacancies) in pristine form. Interestingly, active sites can be effectively engineered within the continuous MoS 2 sheets by treating it with plasma in a controlled manner. Here, we employed N 2 plasma on a large-area continuous-monolayer MoS 2 synthesized via metal-organic chemical vapor deposition to acquire maximum active sites that are indeed required for an efficient HER performance. The MoS 2 samples with maximum active sites were acquired by optimizing the plasma exposure time. The newly induced edges and S-vacancies were directly verified by high-resolution transmission electron microscopy. The 20 min treated MoS 2 sample showed maximum active sites and thereby maximum HER activity, onset overpotential of ∼-210 mV vs reversible hydrogen electrode (RHE), and Tafel slope of ∼89 mV/dec. Clearly, the above results show that this approach can be employed for improving the HER efficiency of large-scale MoS 2 -based electrocatalysts., Competing Interests: The authors declare no competing financial interest., (Copyright © 2019 American Chemical Society.)

Single-crystalline silicon carbide (3C-SiC) on the Si substrate has drawn significant attention in recent years due to its low wafer cost and excellent mechanical, chemical, and optoelectronic properties. However, the applications of the structure have primarily been focused on piezoresistive and pressure sensors, bio-microelectromechanical system, and photonics. Herein, we report another promising application of the heterostructure as a laser spot position-sensitive detector (PSD) based on the lateral photovoltaic effect (LPE) under nonuniform optical illuminations at zero-bias conditions. The LPE shows a linear dependence on spot positions, and the sensitivity is found to be as high as 33 mV/mm under an illumination of 2.8 W/cm 2 (635 nm). The structure also exhibits a linear dependence of the LPE over a large distance (7 mm) between two electrodes, which is crucial for PSDs as the region with a linear dependence of LPE is only usable for PSDs. The LPE at different spot positions and under different illumination conditions have been investigated and explained based on the energy-band analysis. The temperature dependence of the LPE and position sensitivity is also investigated. Furthermore, the two-dimensional mapping of the lateral photovoltages reveals the potential for utilizing the 3C-SiC/Si heterostructure to detect the laser spot position precisely on a plane.

Implantable electronics are of great interest owing to their capability for real-time and continuous recording of cellular-electrical activity. Nevertheless, as such systems involve direct interfaces with surrounding biofluidic environments, maintaining their long-term sustainable operation, without leakage currents or corrosion, is a daunting challenge. Herein, we present a thin, flexible semiconducting material system that offers attractive attributes in this context. The material consists of crystalline cubic silicon carbide nanomembranes grown on silicon wafers, released and then physically transferred to a final device substrate ( e.g. , polyimide). The experimental results demonstrate that SiC nanomembranes with thicknesses of 230 nm do not experience the hydrolysis process ( i.e. , the etching rate is 0 nm/day at 96 °C in phosphate-buffered saline (PBS)). There is no observable water permeability for at least 60 days in PBS at 96 °C and non-Na + ion diffusion detected at a thickness of 50 nm after being soaked in 1× PBS for 12 days. These properties enable Faradaic interfaces between active electronics and biological tissues, as well as multimodal sensing of temperature, strain, and other properties without the need for additional encapsulating layers. These findings create important opportunities for use of flexible, wide band gap materials as essential components of long-lived neurological and cardiac electrophysiological device interfaces.

Conformal growth of atomic-thick semiconductor layers on patterned substrates can boost up the performance of electronic and optoelectronic devices remarkably. However, conformal growth is a very challenging technological task, since the control of the growth processes requires utmost precision. Herein, we report on conformal growth and characterization of monolayer MoS 2 on planar, microrugged, and nanorugged SiO 2 /Si substrates via metal-organic chemical vapor deposition. The continuous and conformal nature of monolayer MoS 2 on the rugged surface was verified by high-resolution transmission electron microscopy. Strain effects were examined by photoluminescence (PL) and Raman spectroscopy. Interestingly, the photoresponsivity (∼254.5 mA/W) of as-grown MoS 2 on the nanorugged substrate was 59 times larger than that of the planar sample (4.3 mA/W) under a small applied bias of 0.1 V. This value is record high when compared with all previous MoS 2 -based photocurrent generation under low or zero bias. Such enhancement in the photoresponsivity arises from a large active area for light-matter interaction and local strain for PL quenching, wherein the latter effect is the key factor and unique in the conformally grown monolayer on the nanorugged surface.

Over the last decades, the spin-coating (SC) technique has been widely used to prepare thin films of various materials in the liquid phase on arbitrary substrates. The technique simply relies on the centrifugal force to spread a coating solution radially outward over the substrate. This mechanism works fairly well for solutions with low surface tension to form thin films of reasonable junctions on smooth substrates. Here, we present a modified SC technique, namely, ultrasonic-assisted spin-coating (UASC), to form thin films of coating solution having high surface tension on rough substrates with excellent junctions. The UASC technique couples SC with an external ultrasonic wave generator to provide external perturbation to locally break down big drops of the coating material into smaller droplets via Rayleigh instability. Because of their lower mass, these tiny droplets gain low momenta and move slowly both in radial and azimuthal directions, giving them an enough time to effectively permeate within pores, thereby yielding excellent junctions. Furthermore, we also investigated the effect of junction improvement on conventional and inverted bulk heterojunction organic solar cells. Intriguingly, the organic solar cells fabricated by the UASC method showed an improved efficiency compared to typical SC owing to efficient charge transfer across the junction. These results clearly imply that UASC is a simple and powerful technique which can significantly enhance the device performance by improving the junction. Moreover, we believe that UASC can be more effective for the preparation of devices composed of multilayers of different materials having complicated nanostructures.

Micromachined membranes are promising platforms for cell culture thanks to their miniaturization and integration capabilities. Possessing chemical inertness, biocompatibility, and integration, silicon carbide (SiC) membranes have attracted great interest toward biological applications. In this paper, we present the batch fabrication, mechanical characterizations, and cell culture demonstration of robust ultrathin epitaxial deposited SiC membranes. The as-fabricated ultrathin SiC membranes, with an ultrahigh aspect ratio (length/thickness) of up to 20 000, possess high a fracture strength up to 2.95 GPa and deformation up to 50 μm. A high optical transmittance of above 80% at visible wavelengths was obtained for 50 nm membranes. The as-fabricated membranes were experimentally demonstrated as an excellent substrate platform for bio-MEMS/NEMS cell culture with the cell viability rate of more than 92% after 72 h. The ultrathin SiC membrane is promising for in vitro observations/imaging of bio-objects with an extremely short optical access.

Single-crystal cubic silicon carbide has attracted great attention for MEMS and electronic devices. However, current leakage at the SiC/Si junction at high temperatures and visible-light absorption of the Si substrate are main obstacles hindering the use of the platform in a broad range of applications. To solve these bottlenecks, we present a new platform of single crystal SiC on an electrically insulating and transparent substrate using an anodic bonding process. The SiC thin film was prepared on a 150 mm Si with a surface roughness of 7 nm using LPCVD. The SiC/Si wafer was bonded to a glass substrate and then the Si layer was completely removed through wafer polishing and wet etching. The bonded SiC/glass samples show a sharp bonding interface of less than 15 nm characterized using deep profile X-ray photoelectron spectroscopy, a strong bonding strength of approximately 20 MPa measured from the pulling test, and relatively high optical transparency in the visible range. The transferred SiC film also exhibited good conductivity and a relatively high temperature coefficient of resistance varying from -12 000 to -20 000 ppm/K, which is desirable for thermal sensors. The biocompatibility of SiC/glass was also confirmed through mouse 3T3 fibroblasts cell-culturing experiments. Taking advantage of the superior electrical properties and biocompatibility of SiC, the developed SiC-on-glass platform offers unprecedented potentials for high-temperature electronics as well as bioapplications.

Infectious diseases remain one of the leading causes of death worldwide despite the tremendous effort devoted to the design and development of antimicrobial agents. However, the decrease in the effectiveness of some antibiotics is often associated with the development of drug resistance by pathogen. This leads to an urgent need for the development of new therapeutic approaches that can overcome the development of drug resistance. Recent evidence suggests that the biological signaling molecule carbon monoxide (CO) presents remarkable antimicrobial properties. Herein, we report the design and synthesis of a new type of water-soluble CO-releasing polymer with antimicrobial activity against Pseudomonas aeruginosa that is highly efficient at preventing biofilm formation.

Water is a ubiquitous and abundant component of atmospheric aerosols. It influences light scattering, the hydrological cycle, atmospheric chemistry, and secondary particulate matter (PM) formation. Despite the critical importance of aerosol liquid water, mass concentrations are not well-known. Using speciated ion and meteorological data from the Southeastern Aerosol Research and Characterization network, we employ the thermodynamic model ISORROPIAv2.1 to estimate water mass concentrations and evaluate trends from 2001 to 2012 in urban and rural locations. The purpose of this study is to better understand the historical trends of aerosol liquid water in the southeast U.S. in the context of improved air quality and recently noted reductions in particulate organic carbon (OC). Aerosol water mass concentrations decrease by ∼79% from 2001 to 2012 in the region. Decreases are more prominent in rural than in urban areas. Fractional contribution of water to PM also decreases during the same time period, and this is consistent with recently noted improvements in visibility. These findings agree with the hypotheses that aerosol liquid water facilitates formation of biogenic secondary organic aerosol (SOA) and that biogenically derived SOA is modulated in the presence of anthropogenic perturbations.

The structural diversity of natural sulfated glycosaminoglycans (GAGs) presents major promise for discovery of chemical biology tools or therapeutic agents. Yet, few GAGs have been identified so far to exhibit this promise. We reasoned that a simple approach to identify such GAGs is to explore sequences containing rare residues, for example, 2-O-sulfonated glucuronic acid (GlcAp2S). Genetic algorithm-based computational docking and filtering suggested that GlcAp2S containing heparan sulfate (HS) may exhibit highly selective recognition of antithrombin, a key plasma clot regulator. HS containing only GlcAp2S and 2-N-sulfonated glucosamine residues, labeled as HS2S2S, was chemoenzymatically synthesized in just two steps and was found to preferentially bind antithrombin over heparin cofactor II, a closely related serpin. Likewise, HS2S2S directly inhibited thrombin but not factor Xa, a closely related protease. The results show that a HS containing rare GlcAp2S residues exhibits the unusual property of selective antithrombin activation and direct thrombin inhibition. More importantly, HS2S2S is also the first molecule to activate antithrombin nearly as well as the heparin pentasaccharide although being completely devoid of the critical 3-O-sulfonate group. Thus, this work shows that novel functions and mechanisms may be uncovered by studying rare GAG residues/sequences.

One of the distinct structural features of many proteoglycans (PGs) is the presence of two or more glycosaminoglycan (GAG) side chains covalently linked to a core protein. Previous studies have shown that the synergistic biological activity of multiple GAG chains, as found in the majority of PGs, cannot be accomplished by the sum of the activities of individual GAG chains. To delineate the biological significance of GAG valency, a number of cluster-xylosides carrying two, three, or four xylose residues on the same scaffold were synthesized using click chemistry. Assessment of cluster-xylosides for their GAG chain priming activity in a cellular system revealed that these cluster-xylosides prime multiple GAG chains per scaffold. Multivalent GAG chains, produced by cluster-xylosides, can better mimic PGs as they carry two or more GAG chains attached to a core protein and therefore can be used as molecular probes to examine the biological significance of GAG multivalency in model organisms.

Proteoglycans (PGs) modulate numerous signaling pathways during development through binding of their glycosaminoglycan (GAG) side chains to various signaling molecules, including fibroblast growth factors (FGFs). A majority of PGs possess two or more GAG side chains, suggesting that GAG multivalency is imperative for biological functions in vivo. However, only a few studies have examined the biological significance of GAG multivalency. In this report, we utilized a library of bis- and tris-xylosides that produce two and three GAG chains on the same scaffold, respectively, thus mimicking PGs, to examine the importance of GAG valency and chain type in regulating FGF/FGFR interactions in vivo in zebrafish. A number of bis- and tris-xylosides, but not mono-xylosides, caused an elongation phenotype upon their injection into embryos. In situ hybridization showed that elongated embryos have elevated expression of the FGF target gene mkp3 but unchanged expression of reporters for other pathways, indicating that FGF/FGFR signaling was specifically hyperactivated. In support of this observation, elongation can be reversed by the tyrosine kinase inhibitor SU5402, mRNA for the FGFR antagonist sprouty4, or FGF8 morpholino. Endogenous GAGs seem to be unaffected after xyloside treatment, suggesting that this is a gain-of-function phenotype. Furthermore, expression of a multivalent but not a monovalent GAG containing syndecan-1 proteoglycan recapitulates the elongation phenotype observed with the bivalent xylosides. On the basis of these in vivo findings, we propose a new model for GAG/FGF/FGFR interactions in which dimerized GAG chains can activate FGF-mediated signal transduction pathways.

The simultaneous Ostwald ripening of an emulsion and the solubilization of its oil droplets by added micellar surfactant solutions are monitored by measurements of time-averaged scattered intensities. A simple computer simulation model for the interpretation of the measurements is presented. Experimental data are analyzed with this model using one single parameter: an effective ratio of oil to surfactant molecules involved in the withdrawal of oil from the Ostwald ripening process by the added micelles. The fitted value of this parameter appears to be more than twice the one that can be predicted from the equilibrium solubilization of oil by the surfactant micelles, indicating that more oil is involved in the nonequilibrium exchange of oil and surfactant between micelles and droplets., (Copyright 2004 American Chemical Society)