Template-Free Preparation of a Mesopore-Rich Hierarchically Porous Carbon Monolith from a Thermally Rearrangeable Polyurea Network.

A mesopore-rich, hierarchically porous carbon monolith was prepared by carbonizing a polyisocyanurate network derived by thermal rearrangement of a polyurea network. The initial polyurea network was synthesized by the cross-linking polymerization of tetrakis(4-aminophenyl)methane (TAPM) and hexamethylene diisocyanate (HDI) in the sol-forming condition, followed by precipitation into nanoparticulate solids in a nonsolvent. The powder was molded into a shape and then heated at 200-400 °C to obtain the porous carbon precursor composed of the rearranged network. The thermolysis of urea bonds to amine and isocyanate groups, the subsequent cyclization of isocyanates to isocyanurates, and the vaporization of volatiles caused sintering of the nanoparticles into a monolithic network with micro-, meso-, and macropores. The rearranged network was carbonized to obtain a carbon monolith. It was found that the rearranged network, with a high isocyanurate ratio, led to a porous carbon with a high mesopore ratio. The electrical conductivity of the resulting carbon monoliths exhibited a rapid response to carbon dioxide adsorption, indicating efficient gas transport through the hierarchical pore structure.

Single-molecule DNA visualization using AT-specific red and non-specific green DNA-binding fluorescent proteins.

The recent advances in the single cell genome analysis are generating a considerable amount of novel insights into complex biological systems. However, there are still technical challenges because each cell has a single copy of DNA to be amplified in most single cell genome analytical methods. In this paper, we present a novel approach to directly visualize a genomic map on a large DNA molecule instantly stained with red and green DNA-binding fluorescent proteins without DNA amplification. For this visualization, we constructed a few types of fluorescent protein-fused DNA-binding proteins: H-NS (histone-like nucleoid-structuring protein), DNA-binding domain of BRCA1 (breast cancer 1), high mobility group-1 (HMG), and lysine tryptophan (KW) repeat motif. Because H-NS and HMG preferentially bind A/T-rich regions, we combined A/T specific binder (H-NS-mCherry and HMG-mCherry as red color) and a non-specific complementary DNA binder (BRCA1-eGFP and 2(KW)2-eGFP repeat as green color) to produce a sequence-specific two-color DNA physical map for efficient optical identification of single DNA molecules.

Enhanced Performance of MoS2 Photodetectors by Inserting an ALD-Processed TiO2 Interlayer.

2D molybdenum disulfide (MoS2 ) possesses excellent optoelectronic properties that make it a promising candidate for use in high-performance photodetectors. Yet, to meet the growing demand for practical and reliable MoS2 photodetectors, the critical issue of defect introduction to the interface between the exfoliated MoS2 and the electrode metal during fabrication must be addressed, because defects deteriorate the device performance. To achieve this objective, the use of an atomic layer-deposited TiO2 interlayer (between exfoliated MoS2 and electrode) is reported in this work, for the first time, to enhance the performance of MoS2 photodetectors. The TiO2 interlayer is inserted through 20 atomic layer deposition cycles before depositing the electrode metal on MoS2 /SiO2 substrate, leading to significantly enhanced photoresponsivity and response speed. These results pave the way for practical applications and provide a novel direction for optimizing the interlayer material.

Fabrication of silica nanostructures with a microwave assisted direct patterning process.

Silica nanostructures were fabricated on glass substrate using a microwave assisted direct patterning (MADP) process, which is a variety of soft lithography. During the MADP process using polydimethylsiloxane (PDMS), mold and microwave heating are performed simultaneously. Blanket thin film and micro- to nano-sized structures, including moth-eye patterns of SiO2, which consisted of coalesced silica nanoparticles, were formed on glass substrates from SiO2 nano-particle dispersed solutions with varied microwave heating time. Optical properties and surface morphologies of micro-sized hemisphere, nano-sized pillar, moth-eye and 50 nm sized line/space silica patterns were measured using UV-vis and a scanning electron microscope. X-ray diffraction analysis of SiO2 thin films with and without microwave heating was also carried out.

Tailoring n-ZnO/p-Si branched nanowire heterostructures for selective photoelectrochemical water oxidation or reduction.

We report the fabrication of three-dimensional (3D) branched nanowire (NW) heterostructures, consisting of periodically ordered vertical Si NW trunks and ZnO NW branches, and their application for solar water splitting. The branched NW photoelectrodes show orders of magnitudes higher photocurrent compared to the bare Si NW electrodes. More interestingly, selective photoelectrochemical cathodic or anodic behavior resulting in either solar water oxidation or reduction was achieved by tuning the doping concentration of the p-type Si NW core. Specifically, n-ZnO/p-Si branched NW array electrodes with lightly doped core show broadband absorption from UV to near IR region and photocathodic water reduction, while n-ZnO/p(+)-Si branched NW arrays show photoanodic water oxidation with photoresponse only to UV light. The photoelectrochemical stability for over 24 h under constant light illumination and fixed biasing potential was achieved by coating the branched NW array with thin layers of TiO2 and Pt. These studies not only reveal the promise of 3D branched NW photoelectrodes for high efficiency solar energy harvesting and conversion to clean chemical fuels, but also developing understanding enabling rational design of high efficiency robust photocathodes and photoanodes from low-cost and earth-abundant materials allowing practical applications in clean renewable energy.

Monolithic Perovskite-Silicon Dual-Band Photodetector for Efficient Spectral Light Discrimination.

Selective spectral discrimination of visible and near-infrared light, which accurately distinguishes different light wavelengths, holds considerable promise in various fields, such as automobiles, defense, and environmental monitoring. However, conventional imaging technologies suffer from various issues, including insufficient spatial optimization, low definition, and optical loss. Herein, a groundbreaking advancement is demonstrated in the form of a dual-band photodiode with distinct near-infrared- and visible-light discrimination obtained via simple voltage control. The approach involves the monolithic stacking integration of methylammonium lead iodide (MAPbI3) and Si semiconductors, resulting in a p-Si/n-phenyl-C61-butyric acid methyl ester/i-MAPbI3/p-spiro-MeOTAD (PNIP) device. Remarkably, the PNIP configuration can independently detect the visible and near-infrared regions without traditional optical filters under a voltage range of 3 to -3 V. In addition, an imaging system for a prototype autonomous vehicle confirms the capability of the device to separate visible and near-infrared light via an electrical bias and practicality of this mechanism. Therefore, this study pushes the boundaries of image sensor development and sets the stage for fabricating compact and power-efficient photonic devices with superior performance and diverse functionality.

Efficiency enhancement of white light-emitting diodes via nano-textured silicone encapsulant.

We textured the surface of a silicone encapsulant to increase the extraction efficiency of white light-emitting diodes (LEDs) by using a plasma treatment. Here, the surface morphology could be controlled by changing the plasma condition and texturing morphology of the silicone encapsulant were proportion to the increased ratio of white LEDs. The luminous efficacy of the surface textured LEDs were increased 9.70% relative to the reference LED. Furthermore, the Fourier transform infrared spectroscopy spectrum showed that the chemical bonds of the silicone encapsulant were not changed by the argon-nitrogen plasma treatment, thereby reducing degradation of the optical characteristics and improving the reliability of LEDs.

Probing the lithium ion storage properties of positively and negatively carved silicon.

Here, we report Si pillar and well arrays as tailored electrode materials for advanced Li ion storage devices. The well-ordered and periodic morphologies were formed on a Si electrode thin film via laser interference lithography followed by a dry etch process. Two different patterns of negatively or positively carved Si electrodes exhibited highly improved cycle performance as a consequence of the enlarged surface area and the nanoscale pattern effects. The Si well arrays showed the highest energy density, rate capability, and cycling retention among the prepared Si electrodes. This tailored electrode platform demonstrates that these design principles could be applied to future developments in Si electrodes.

Perovskite multifunctional logic gates via bipolar photoresponse of single photodetector.

The explosive demand for a wide range of data processing has sparked interest towards a new logic gate platform as the existing electronic logic gates face limitations in accurate and fast computing. Accordingly, optoelectronic logic gates (OELGs) using photodiodes are of significant interest due to their broad bandwidth and fast data transmission, but complex configuration, power consumption, and low reliability issues are still inherent in these systems. Herein, we present a novel all-in-one OELG based on the bipolar spectral photoresponse characteristics of a self-powered perovskite photodetector (SPPD) having a back-to-back p+-i-n-p-p+ diode structure. Five representative logic gates ("AND", "OR", "NAND", "NOR", and "NOT") are demonstrated with only a single SPPD via the photocurrent polarity control. For practical applications, we propose a universal OELG platform of integrated 8 × 8 SPPD pixels, demonstrating the 100% accuracy in five logic gate operations irrelevant to current variation between pixels.

A crossbar-type high sensitivity ultraviolet photodetector array based on a one hole-one nanorod configuration via nanoimprint lithography.

Single crystalline vertical ZnO nanorods were grown in a one hole-one rod configuration using a hydrothermal method with a patterned polymer template generated by nanoimprint lithography, allowing precise control over the position and density of the ZnO nanorods. An 8×8 ZnO nanorod-based ultraviolet photodetector array is demonstrated, in which a well-confined number of ZnO nanorods are sandwiched between crossbar-type platinum and indium tin oxide electrodes (e.g. 16 nanorods in a 2×2 µm2 area). A high photocurrent/dark current ratio of 3×10(3) at a reverse bias of 1.5 V under UV illumination at room temperature, a responsivity of 4381.4 A W(-1) at 365 nm, and an ultraviolet-to-visible rejection ratio of 83 are obtained and maintained, irrespective of pixel size. A uniform photoresponse is achieved in each of the pixels, indicating the scalability with this technique for fabricating an integrated UV photodetector array circuit.

Fabrication of silicon nanowire for detecting p-amyloid (1-42) by nanoimprint lithography.

Ultraviolet nanoimprint lithography (UV-NIL) is a high volume and cost-effective patterning technique with sub-10 nm resolution. It has great potential as a candidate for next generation lithography. Using UV-NIL, nanowire patterns were successfully fabricated on a four-inch silicon-on-insulator (SOI) wafer under moderate conditions. The fabricated nanowire patterns were characterized by FE-SEM. Its electrical properties were confirmed by semiconductor parameter analysis. Monoclonal antibodies against beta-amyloid (1-42) were immobilized on the silicon nanowire using a chemical linker. Using this fabricated silicon nanowire device, beta-amyloid (1-42) levels of 1 pM to 100 nM were successfully determined from conductance versus time characteristics. Consequently, the nanopatterned SOI nanowire device can be applied to bioplatforms for the detection of proteins.

Omni-directional wind-driven triboelectric nanogenerator with cross-shaped dielectric film.

Triboelectric nanogenerators (TENGs) are actively being researched and developed to become a new external power unit for various electronics and applications. Wind is proposed as a mechanical energy source to flutter the dielectric film in wind-driven TENGs as it is clean, abundant, ubiquitous, and sustainable. Herein, we propose a TENG structure with dielectric films bent in four directions to collect the wind energy supply from all directions, unlike the conventional wind-driven TENGs which can only harvest the wind energy from one direction. Aluminum (Al) layer was intercalated within the dielectric film to improve electrostatic induction, resulting in improved triboelectric performances. Maximum open-circuit voltage (Voc) of 233 V, short-circuit current (Isc) of 348 µA, and output power density of 46.1 W m- 2 at an external load of 1 MΩ under a wind speed of 9 m s- 1 were revealed, and it faithfully lit "LED" characters composed of 25 LEDs.

Design of Chemically Stable Organic Perovskite Quantum Dots for Micropatterned Light-Emitting Diodes through Kinetic Control of a Cross-Linkable Ligand System.

Perovskite quantum dot (QD) light-emitting diodes (PeLEDs) are ideal for next-generation display applications because of their excellent color purity, high efficiency, and cost-effective fabrication. However, developing a technology for high-resolution multicolor patterning of perovskite QDs remains challenging, owing to the chemical instability of these materials. To overcome these issues, in this work, the generation of surface defects is prevented by controlling the ligand-binding kinetics using a stable ligand system (Stable LS). The crystalline reconstruction of perovskite QDs after addition of the Stable LS results in an ≈18% increase in their photoluminescence quantum yield in solution and it also improves the ambient stability of the perovskite QD solution. Moreover, the perovskite QDs with Stable LS can undergo cross-linking under UV irradiation. The tightly bridged perovskite QDs effectively prevent moisture-assisted ligand dissociation in film state due to the increased hydrophobicity and restricted movement of the cross-linked surface ligands. Thus, the cross-linked perovskite QD film shows improved chemical/environmental stability without substantial deterioration in optoelectrical properties. As a result, a white electroluminescent device with high resolution (≈1 µm) is successfully fabricated by inkjet printing using green and red perovskite QDs.

Reactant/polymer hybrid films on p-n junction photodetectors for self-powered, non-invasive glucose biosensors.

The portability of electronic-based biosensors is limited because of the use of batteries and/or solutions containing reactants such as enzymes for assay, which limits the utility of such biosensors in point-of-care (POC) testing. In this study, we report on the development of a self-powered biosensor composed of only portable components: a reactant-containing poly (ethylene glycol) (PEG) film for the colorimetric assay, and a self-powered n-InGaZnO/p-Si photodetector. The PEG film containing enzymes and color-developing agents was formed on a glass slide by spin coating. The self-powered biosensor was fabricated by placing the hybrid film on the p-n junction photodetector, and applied in non-invasive glucose detection (salivary glucose). Injection of the target-containing solution dissolved the PEG that led to the release of enzymes and color-developing agents, resulting in a colorimetric assay. The colorimetric assay could attenuate the light reaching the photodetector, thus facilitating target concentration verification by measuring the photocurrent. Our self-powered biosensor has two main advantages: (i) all components of the biosensor are portable and (ii) dilution of target concentration is avoided as the reagents are in the PEG film. Therefore, the self-powered biosensor, without solution-phase components, could be highly beneficial for creating portable, sensitive biosensors for POC testing.

Sandwich-Doping for a Large Schottky Barrier and Long-Term Stability in Graphene/Silicon Schottky Junction Solar Cells.

Doping is an effective method for controlling the electrical properties and work function of graphene which can improve the power conversion efficiency of graphene-based Schottky junction solar cells (SJSCs). However, in previous approaches, the stability of chemical doping decreased over time due to the decomposition of dopants on the surface of graphene under ambient conditions. Here, we report an efficient and strong p-doping by simple sandwich doping on both the top and bottom surfaces of graphene. We confirmed that the work function of sandwich-doped graphene increased by 0.61 eV and its sheet resistance decreased by 305.8 Ω/sq, compared to those of the pristine graphene. Therefore, the graphene-silicon SJSCs that used sandwich-doped graphene had a power conversion efficiency of 10.02%, which was 334% higher than that (2.998%) of SJSCs that used pristine graphene. The sandwich-doped graphene-based silicon SJSCs had excellent long-term stability over 45 days without additional encapsulation.

Molecular Sieve Based on a PMMA/ZIF-8 Bilayer for a CO-Tolerable H2 Sensor with Superior Sensing Performance.

Semiconductor sensors equipped with Pd catalysts are promising candidates as low-powered and miniaturized surveillance devices that are used to detect flammable hydrogen (H2) gas. However, the following issues remain unresolved: (i) a sluggish sensing speed at room temperature and (ii) deterioration of sensing performance caused by interfering gases, particularly, carbon monoxide (CO). Herein, a bilayer comprising poly(methyl methacrylate) (PMMA) and zeolitic imidazolate framework-8 (ZIF-8) is utilized as a molecular sieve for diode-type H2 sensors based on a Pd-decorated indium-gallium-zinc oxide film on a p-type silicon substrate. While the PMMA effectively blocks the penetration of CO gas molecules into the sensing entity, the ZIF-8 improves sensing performances by modifying the catalytic activity of Pd, which is preferable for splitting H2 and O2 molecules. Consequently, the bilayer-covered sensor achieves outstanding CO tolerance with superior sensing figures of merit (response/recovery times of <10 s and sensing response of >5000% at 1% H2).

High-Performance Photovoltaic Hydrogen Sensing Platform with a Light-Intensity Calibration Module.

Although battery-free gas sensors (e.g., photovoltaic or triboelectric sensors) have recently appeared to resolve the power consumption issue of conventional chemiresistors, severe technical barriers still remain. Especially, their signals varying under ambient conditions such as light intensity restrict the utilization of these sensors. Insufficient sensing performances (low response and slow sensing rate) of previous battery-free sensors are also an obstacle for practical use. Herein, a photovoltaic hydrogen (H2)-sensing platform having constant sensing responses regardless of light conditions is demonstrated. The platform consists of two photovoltaic units: (1) a palladium (Pd)-decorated n-IGZO/p-Si photodiode covered with a microporous zeolitic imidazolate framework-8 (ZIF-8) film and (2) a device with the same configuration, but without the Pd catalyst as a reference to calibrate the base current of sensor (1). The platform after calibration yields accurate response values in real time regardless of unknown irradiance. Besides, the sensing performances (e.g., sensing response of 1.57 × 104% at 1% H2 with a response time <15 s) of our platform are comparable with those of the conventional resistive H2 sensors, which yield unprecedented results in photovoltaic H2 sensors.

Enhancement of Interfacial Adhesion Using Micro/Nanoscale Hierarchical Cilia for Randomly Accessible Membrane-Type Electronic Devices.

The recent technology of transfer printing using various membrane-type flexible/stretchable electronic devices can provide electronic functions to desirable objects where direct device fabrication is difficult. However, if the target surfaces are rough and complex, the capability of accommodating surface mismatches for reliable interfacial adhesion remains a challenge. Here, we demonstrate that newly designed nanotubular cilia (NTCs), vertically aligned underneath a polyimide substrate, significantly enhance interfacial adhesion. The tubular structure easily undergoes flattening and wrapping motions to provide a large conformal contact area, and the synergetic effect of the assembled cilia strengthens the overall adhesion. Furthermore, the hierarchical structure consisting of radially spread film-type cilia combined with vertically aligned NTCs in specific regions enables successful transfer printing onto very challenging surfaces such as stone, bark, and textiles. Finally, we successfully transferred a temperature sensor onto an eggshell and indium gallium zinc oxide-based transistors onto a stone with no electrical failure.

Gold nanocap-supported upconversion nanoparticles for fabrication of a solid-phase aptasensor to detect ochratoxin A.

Solid-phase, single-step biosensors are crucial for the development of portable, reusable, and convenient biosensors, otherwise known as point-of-care (POC) testing. Although high-performance single-step biosensors based on the principle of Förster resonance energy transfer (FRET) and using upconversion nanoparticles (UCNPs) functionalized with aptamers have been suggested as easy-to-use platforms, they lack portability and reusability when used for solution-phase biosensing. In this study, we describe a solid-phase, single-step aptasensor that showed higher performance than those of solution-phase aptasensors, as well as promising reusability. The solid-phase, single-step aptasensor was developed based on Au nanocap-supported UCNPs (Au/UCNPs), which were partially embedded in a solid substrate (e.g. polydimethylsiloxane, PDMS). The Au nanocaps allowed the UCNPs to emit upconverted light only from the restricted areas of the UCNPs, i.e., where they were not covered by the nanocaps and PDMS. Functionalization of an aptamer labeled with a quencher on the restricted area enabled the effective quenching of upconverted light from Au/UCNP via FRET after target (ochratoxin A, OTA) detection. The solid-phase, single-step aptasensor showed a linear range of 0.1-1000 ng mL-1 and limit of detection of 0.022 ng mL-1 within 30 min toward OTA. Furthermore, reusability of the solid-phase aptasensor was evaluated for three cycles of detection and regeneration, establishing its apparent reusability via heat treatment. Hence, such solid-phase, single-step aptasensors pave the path to the development of a portable and reusable biosensor platform for POC testing.

Small extracellular vesicles from human adipose-derived stem cells attenuate cartilage degeneration.

Osteoarthritis (OA) is a chronic degenerative disease of articular cartilage that is the most common joint disease worldwide. Mesenchymal stem cells (MSCs) have been the most extensively explored for the treatment of OA. Recently, it has been demonstrated that MSC-derived extracellular vesicles (EVs) may contribute to the potential mechanisms of MSC-based therapies. In this study, we investigated the therapeutic potential of human adipose-derived stem cells EVs (hASC-EVs) in alleviating OA, along with the mechanism. EVs were isolated from the culture supernatants of hASCs by a multi-filtration system based on the tangential flow filtration (TFF) system. The isolated EVs were characterised using dynamic light scattering (DLS), transmission electron microscopy (TEM), nanoparticle tracking analysis (NTA) and flow cytometry analysis. The hASC-EVs not only promoted the proliferation and migration of human OA chondrocytes, but also maintained the chondrocyte matrix by increasing type Ⅱ collagen synthesis and decreasing MMP-1, MMP-3, MMP-13 and ADAMTS-5 expression in the presence of IL-1ß in vitro. Intra-articular injection of hASC-EVs significantly attenuated OA progression and protected cartilage from degeneration in both the monosodium iodoacetate (MIA) rat and the surgical destabilisation of the medial meniscus (DMM) mouse models. In addition, administration of hASC-EVs inhibited the infiltration of M1 macrophages into the synovium. Overall results suggest that the hASC-EVs should be considered as a potential therapeutic approach in the treatment of OA.