Float-stacked graphene-PMMA laminate.

Semi-infinite single-atom-thick graphene is an ideal reinforcing material that can simultaneously improve the mechanical, electrical, and thermal properties of matrix. Here, we present a float-stacking strategy to accurately align the monolayer graphene reinforcement in polymer matrix. We float graphene-poly(methylmethacrylate) (PMMA) membrane (GPM) at the water-air interface, and wind-up layer-by-layer by roller. During the stacking process, the inherent water meniscus continuously induces web tension of the GPM, suppressing wrinkle and folding generation. Moreover, rolling-up and hot-rolling mill process above the glass transition temperature of PMMA induces conformal contact between each layer. This allows for pre-tension of the composite, maximizing its reinforcing efficiency. The number and spacing of the embedded graphene fillers are precisely controlled. Notably, we accurately align 100 layers of monolayer graphene in a PMMA matrix with the same intervals to achieve a specific strength of about 118.5 MPa g-1 cm3, which is higher than that of lightweight Al alloy, and a thermal conductivity of about 4.00 W m-1 K-1, which is increased by about 2,000 %, compared to the PMMA film.

All-Solution-Processed High-Performance MoS2 Thin-Film Transistors with a Quasi-2D Perovskite Oxide Dielectric.

Assembling solution-processed van der Waals (vdW) materials into thin films holds great promise for constructing large-scale, high-performance thin-film electronics, especially at low temperatures. While transition metal dichalcogenide thin films assembled in solution have shown potential as channel materials, fully solution-processed vdW electronics have not been achieved due to the absence of suitable dielectric materials and high-temperature processing. In this work, we report on all-solution-processedvdW thin-film transistors (TFTs) comprising molybdenum disulfides (MoS2) as the channel and Dion-Jacobson-phase perovskite oxides as the high-permittivity dielectric. The constituent layers are prepared as colloidal solutions through electrochemical exfoliation of bulk crystals, followed by sequential assembly into a semiconductor/dielectric heterostructure for TFT construction. Notably, all fabrication processes are carried out at temperatures below 250 °C. The fabricated MoS2 TFTs exhibit excellent device characteristics, including high mobility (>10 cm2 V-1 s-1) and an on/off ratio exceeding 106. Additionally, the use of a high-k dielectric allows for operation at low voltage (∼5 V) and leakage current (∼10-11 A), enabling low power consumption. Our demonstration of the low-temperature fabrication of high-performance TFTs presents a cost-effective and scalable approach for heterointegrated thin-film electronics.

Selective Laser-Assisted Direct Synthesis of MoS2 for Graphene/MoS2 Schottky Junction.

Implementing a heterostructure by vertically stacking two-dimensional semiconductors is necessary for responding to various requirements in the future of semiconductor technology. However, the chemical-vapor deposition method, which is an existing two-dimensional (2D) material-processing method, inevitably causes heat damage to surrounding materials essential for functionality because of its high synthesis temperature. Therefore, the heterojunction of a 2D material that directly synthesized MoS2 on graphene using a laser-based photothermal reaction at room temperature was studied. The key to the photothermal-reaction mechanism is the difference in the photothermal absorption coefficients of the materials. The device in which graphene and MoS2 were vertically stacked using a laser-based photothermal reaction demonstrated its potential application as a photodetector that responds to light and its stability against cycling. The laser-based photothermal-reaction method for 2D materials will be further applied to various fields, such as transparent display electrodes, photodetectors, and solar cells, in the future.

From Pristine to Heteroatom-Doped Graphene Quantum Dots: An Essential Review and Prospects for Future Research.

Graphene quantum dots (GQDs) are carbon-based zero-dimensional materials that have received considerable scientific interest due to their exceptional optical, electrical, and optoelectrical properties. Their unique electronic band structures, influenced by quantum confinement and edge effects, differentiate the physical and optical characteristics of GQDs from other carbon nanostructures. Additionally, GQDs can be synthesized using various top-down and bottom-up approaches, distinguishing them from other carbon nanomaterials. This review discusses recent advancements in GQD research, focusing on their synthesis and functionalization for potential applications. Particularly, various methods for synthesizing functionalized GQDs using different doping routes are comprehensively reviewed. Based on previous reports, current challenges and future directions for GQDs research are discussed in detail herein.

Self-powered image array composed of touch-free sensors fabricated with semiconductor nanowires.

We successfully develop a self-powered image array (IA) composed of 16 touch-free sensors (TFSs) fabricated with semiconductor InN nanowires (NWs) as a response medium. Without using a power supply, the InN-NW TFS can detect the position of a human hand 30 cm away from the device surface. It also distinguishes different materials such as polyimide, Al foil, printing paper, latex, and polyvinyl chloride in non-contact mode at a distance of 1 cm. The self-powered TFS-IA clearly distinguishes square-shaped transparent polydimethylsiloxane film attached to the back of a human hand positioned 5 cm from the device, indicating the possibility for detecting changes in the surface texture of human skin, such as skin burns or skin cancer. The performance of the self-powered TFS and TFS-IA is attributed to high electrostatic induction of InN NWs by external triboelectricity resulting from the simple movement of the target object, which differs markedly from conventional sensors designed to detect variations in the temperature or light essentially using a power supply.

Integration of multiple electronic components on a microfibre towards an emerging electronic textile platform.

Electronic fibres have been considered one of the desired device platforms due to their dimensional compatibility with fabrics by weaving with yarns. However, a precise connecting process between each electronic fibre is essential to configure the desired electronic circuits or systems. Here, we present an integrated electronic fibre platform by fabricating electronic devices onto a one-dimensional microfibre substrate. Electronic components such as transistors, inverters, ring oscillators, and thermocouples are integrated together onto the outer surface of a fibre substrate with precise semiconductor and electrode patterns. Our results show that electronic components can be integrated on a single fibre with reliable operation. We evaluate the electronic properties of the chip on the fibre as a multifunctional electronic textile platform by testing their switching and data processing, as well as sensing or transducing units for detecting optical/thermal signals. The demonstration of the electronic fibre suggests significant proof of concepts for the realization of high performance with wearable electronic textile systems.

Photothermally Crumpled MoS2 Film as an Omnidirectionally Stretchable Platform.

Molybdenum disulfide (MoS2 ) is considered a fascinating material for next-generation semiconducting applications due to its outstanding mechanical stability and direct transition characteristics comparable to silicon. However, its application to stretchable platforms still is a challenging issue in wearable logic devices and sensors with noble form-factors required for future industry. Here, an omnidirectionally stretchable MoS2 platform with laser-induced strained structures is demonstrated. The laser patterning induces the pyrolysis of MoS2 precursors as well as the weak adhesion between Si and SiO2 layers. The photothermal expansion of the Si layer results in the crumpling of SiO2 and MoS2 layers and the field-effect transistors with the crumpled MoS2 are found to be suitable for strain sensor applications. The electrical performance of the crumpled MoS2 depends on the degree of stretching, showing the stable omnidirectional stretchability up to 8% with approximately four times higher saturation current than its initial state. This platform is expected to be applied to future electronic devices, sensors, and so on.

Two-Dimensional Stacked Composites of Self-Assembled Alkane Layers and Graphene for Transparent Gas Barrier Films with Low Permeability.

Self-assembled alkane layers are introduced between graphene layers to physically block nanometer size defects in graphene and lateral gas pathways between graphene layers. A well-defined hexatriacontane (HTC) monolayer on graphene could cover nanometer-size defects because of the flexible nature and strong intermolecular van der Waals interactions of alkane, despite the roughness of graphene. In addition, HTC multilayers between graphene layers greatly improve their adhesion. This indicates that HTC multilayers between graphene layers can effectively block the lateral pathway between graphene layers by filling open space with close-packed self-assembled alkanes. By these mechanisms, alternately stacked composites of graphene and self-assembled alkane layers greatly increase the gas-barrier property to a water vapor transmission rate (WVTR) as low as 1.2 × 10-3 g/(m2 day), whereas stacked graphene layers generally show a WVTR < 0.5 g/(m2 day). Furthermore, the self-assembled alkane layers have superior crystallinity and wide bandgap, so they have little effect on the transmittance.

Structure-controllable growth of nitrogenated graphene quantum dots via solvent catalysis for selective C-N bond activation.

Photophysical and photochemical properties of graphene quantum dots (GQDs) strongly depend on their morphological and chemical features. However, systematic and uniform manipulation of the chemical structures of GQDs remains challenging due to the difficulty in simultaneous control of competitive reactions, i.e., growth and doping, and the complicated post-purification processes. Here, we report an efficient and scalable production of chemically tailored N-doped GQDs (NGs) with high uniformity and crystallinity via a simple one-step solvent catalytic reaction for the thermolytic self-assembly of molecular precursors. We find that the graphitization of N-containing precursors during the formation of NGs can be modulated by intermolecular interaction with solvent molecules, the mechanism of wh ich is evidenced by theoretical calculations and various spectroscopic analyses. Given with the excellent visible-light photoresponse and photocatalytic activity of NGs, it is expected that the proposed approach will promote the practical utilization of GQDs for various applications in the near future.

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.

Hierarchical Porous Film with Layer-by-Layer Assembly of 2D Copper Nanosheets for Ultimate Electromagnetic Interference Shielding.

The emergence of technologies, such as 5G telecommunication, electric vehicles, and wearable electronics, has prompted demand for ultrahigh-performance and cost-effective shielding materials to protect against both the potentially harmful effects of electromagnetic interference (EMI) on human health and electronic device operation. Here, we report hierarchical porous Cu foils via an assembly of single-crystalline, nanometer-thick, and micrometer-long copper nanosheets and their use in EMI shielding. Layer-by-layer assembly of Cu nanosheets enabled the formation of a hierarchically structured porous Cu film with features such as multilayer stacking; two-dimensional networking; and a layered, sheetlike void architecture. The hierarchical-structured porous Cu foil exhibited outstanding EMI shielding performance compared to the same thickness of dense copper and other materials, exhibiting EMI shielding effectiveness (SE) values of 100 and 60.7 dB at thicknesses of 15 and 1.6 µm, respectively. In addition, the EMI SE of the hierarchical porous Cu film was maintained up to 18 months under ambient conditions at room temperature and showed negligible changes after thermal annealing at 200 °C for 1 h. These findings suggest that Cu nanosheets and their layer-by-layer assembly are one of the promising EMI shielding technologies for practical electronic applications.

Layer-Selective Synthesis of MoS2 and WS2 Structures under Ambient Conditions for Customized Electronics.

Transition metal dichalcogenides (TMDs) have attracted significant interest as one of the key materials in future electronics such as logic devices, optoelectrical devices, and wearable electronics. However, a complicated synthesis method and multistep processes for device fabrication pose major hurdles for their practical applications. Here, we introduce a direct and rapid method for layer-selective synthesis of MoS2 and WS2 structures in wafer-scale using a pulsed laser annealing system (λ = 1.06 µm, pulse duration ∼100 ps) in ambient conditions. The precursor layer of each TMD, which has at least 3 orders of magnitude higher absorption coefficient than those of neighboring layers, rigorously absorbed the incoming energy of the laser pulse and rapidly pyrolyzed in a few nanoseconds, enabling the generation of a MoS2 or WS2 layer without damaging the adjacent layers of SiO2 or polymer substrate. Through experimental and theoretical studies, we establish the underlying principles of selective synthesis and optimize the laser annealing conditions, such as laser wavelength, output power, and scribing speed, under ambient condition. As a result, individual homostructures of patterned MoS2 and WS2 layers were directly synthesized on a 4 in. wafer. Moreover, a consecutive synthesis of the second layer on top of the first synthesized layer realized a vertically stacked WS2/MoS2 heterojunction structure, which can be treated as a cornerstone of electronic devices. As a proof of concept, we demonstrated the behavior of a MoS2-based field-effect transistor, a skin-attachable motion sensor, and a MoS2/WS2-based heterojunction diode in this study. The ultrafast and selective synthesis of the TMDs suggests an approach to the large-area/mass production of functional heterostructure-based electronics.

Direct Synthesis of a Self-Assembled WSe2 /MoS2 Heterostructure Array and its Optoelectrical Properties.

Functional van der Waals heterojunctions of transition metal dichalcogenides are emerging as a potential candidate for the basis of next-generation logic devices and optoelectronics. However, the complexity of synthesis processes so far has delayed the successful integration of the heterostructure device array within a large scale, which is necessary for practical applications. Here, a direct synthesis method is introduced to fabricate an array of self-assembled WSe2 /MoS2 heterostructures through facile solution-based directional precipitation. By manipulating the internal convection flow (i.e., Marangoni flow) of the solution, the WSe2 wires are selectively stacked over the MoS2 wires at a specific angle, which enables the formation of parallel- and cross-aligned heterostructures. The realized WSe2 /MoS2 -based p-n heterojunction shows not only high rectification (ideality factor: 1.18) but also promising optoelectrical properties with a high responsivity of 5.39 A W-1 and response speed of 16 µs. As a feasible application, a WSe2 /MoS2 -based photodiode array (10 × 10) is demonstrated, which proves that the photosensing system can detect the position and intensity of an external light source. The solution-based growth of hierarchical structures with various alignments could offer a method for the further development of large-area electronic and optoelectronic applications.

Two-in-One Device with Versatile Compatible Electrical Switching or Data Storage Functions Controlled by the Ferroelectricity of P(VDF-TrFE) via Photocrosslinking.

Organic electronics demand new platforms that can make integrated circuits and undergo mass production while maintaining diverse functions with high performance. The field-effect transistor has great potential to be a multifunctional device capable of sensing, data processing, data storage, and display. Currently, transistor-based devices cannot be considered intrinsic multifunctional devices because all installed functions are mutually coupled. Such incompatibilities are a crucial barrier to developing an all-in-one multifunctional device capable of driving each function individually. In this study, we focus on the decoupling of electric switching and data storage functions in an organic ferroelectric memory transistor. To overcome the incompatibility of each function, the high permittivity needed for electrical switching and the ferroelectricity needed for data storage become compatible by restricting the motion of poly(vinylidene fluoride-trifluoroethylene) via photocrosslinking with bis-perfluorobenzoazide. The two-in-one device consisting of a photocrosslinked ferroelectric layer exhibits reversible and individual dual-functional operation as a typical transistor with nonvolatile memory. Moreover, a p-MOS depletion load inverter composed of the two transistors with different threshold voltages is also demonstrated by simply changing only one of the threshold voltages by polarization switching. We believe that the two-in-one device will be considered a potential component of integrated organic logic circuits, including memory, in the future.

Rare-Earth-Element-Ytterbium-Substituted Lead-Free Inorganic Perovskite Nanocrystals for Optoelectronic Applications.

Lead-(Pb-) halide perovskite nanocrystals (NCs) are interesting nanomaterials due to their excellent optical properties, such as narrow-band emission, high photoluminescence (PL) efficiency, and wide color gamut. However, these NCs have several critical problems, such as the high toxicity of Pb, its tendency to accumulate in the human body, and phase instability. Although Pb-free metal (Bi, Sn, etc.) halide perovskite NCs have recently been reported as possible alternatives, they exhibit poor optical and electrical properties as well as abundant intrinsic defect sites. For the first time, the synthesis and optical characterization of cesium ytterbium triiodide (CsYbI3 ) cubic perovskite NCs with highly uniform size distribution and high crystallinity using a simple hot-injection method are reported. Strong excitation-independent emission and high quantum yields for the prepared NCs are verified using photoluminescence measurements. Furthermore, these CsYbI3 NCs exhibit potential for use in organic-inorganic hybrid photodetectors as a photoactive layer. The as-prepared samples exhibit clear on-off switching behavior as well as high photoresponsivity (2.4 × 103 A W-1 ) and external quantum efficiency (EQE, 5.8 × 105 %) due to effective exciton dissociation and charge transport. These results suggest that CsYbI3 NCs offer tremendous opportunities in electronic and optoelectronic applications, such as chemical sensors, light emitting diodes (LEDs), and energy conversion and storage devices.

Low-Voltage Organic Transistor Memory Fiber with a Nanograined Organic Ferroelectric Film.

Wearable technology offers new ways to be more proactive about our health and surroundings in real time. For next-generation wearable systems, robust storage and recording media are required to monitor and process the essential electrical signals generated under various unpredictable strain conditions. Here, we report the first fibriform organic transistor memory integrated on a thin and flexible metal wire. A capillary tube coating system allows the formation of a thin and nanograined organic ferroelectric film on the wire. The uniform morphology imparts excellent switching stability (∼100 cycles), quasi-permanent retention (over 5 × 104 s), and low-voltage operation (below 5 V) to the fiber-shaped memory devices. When sewn in a stretchable textile fabric, the memory fiber achieves long retention time of more than 104 s with negligible degradation of memory window even under a constant diagonal strain of 100% that exhibits reliable data storage under tough environments. These results illustrate the possibility of the practical, wearable fiber memory for recording electronic signals in smart garment applications.

Coherence in defect evolution data for the ion beam irradiated graphene.

The defect evolution in graphene produced by ion beam bombardment is investigated by changing the ion species, irradiation energy and dose. Raman spectroscopy is performed to examine the defect yield produced under various ion beam bombardment conditions. The defect yields of the vacancy-type defect are well described by the linear energy transfer (L) and dose (d). By increasing Ld, the defect yields exhibit similar behaviours for all ion species. As a consequence, all the defect yields can be collapsed into a single curve by multiplying them by a single parameter, suggesting that the defect evolution under various ion beam bombardment conditions can be described in a simple formula.

Hybrid dielectrics composed of Al2O3 and phosphonic acid self-assembled monolayers for performance improvement in low voltage organic field effect transistors.

Low voltage operational organic transistors (< 4 V) based on pentacene were successfully fabricated with hybrid dielectric films composed of aluminum oxide using atomic layer deposition and various phosphonic acid-based self-assembled monolayers as the gate dielectrics. High capacitances up to 279 nF/cm2, low leakage current densities of 10-8 A/cm2 at 6 V, and high breakdown fields up to 7.5 MV/cm were obtained. The transistors with the octadecylphosphonic acid hybrid dielectric exhibited an improved saturation mobility of 0.58 cm2/Vs, a subthreshold slope of 151 mV/decade, a threshold voltage of - 1.84 V and an on-off current ratio of 106. The low surface energies of the self-assembled monolayers having non-polar terminal groups, such as methyl and pentafluorophenoxy, improved the carrier conduction of the transistors due to the pentacene growth with an edge-on orientation for low voltage operation. The pentafluorophenoxy end-group showed an accumulation of holes at the semiconductor-dielectric interface.

Enhancement of Adsorption Performance for Organic Molecules by Combined Effect of Intermolecular Interaction and Morphology in Porous rGO-Incorporated Hydrogels.

In this study, we developed reduced graphene oxide (rGO)-incorporated porous agarose (Ar-rGO) composites that were prepared via a "one-pot" sol-gel method involving a mixing and vacuum freeze-drying process. These composites represent an easy-to-use adsorbent for organic contaminant removal. Ar-rGOs can efficiently adsorb organic molecules, especially aromatic organic compounds from wastewater, because of the synergistic effect between the agarose bundles, which function as a water absorption site, and the rGO sheets, which function as active sites for pollutant binding. The pore structures and morphology of the Ar-rGO composites varied according to the added rGO, resulting in effective water infiltration into the composites. The main adsorption mechanism of the aromatic organic compounds onto Ar-rGOs involved π-π interactions with the rGO sheets. The surface interaction was more effective for adsorbing/desorbing the aromatic pollutants than the electrostatic interaction via the O-containing functional groups. In addition, we confirmed that Ar-rGO is highly stable over the entire pH range (1-13) because of the presence of the rGO sheets.

Ultrastrong Graphene-Copper Core-Shell Wires for High-Performance Electrical Cables.

Recent development in mobile electronic devices and electric vehicles requires electrical wires with reduced weight as well as enhanced stability. In addition, since electric energy is mostly generated from power plants located far from its consuming places, mechanically stronger and higher electric power transmission cables are strongly demanded. However, there has been no alternative materials that can practically replace copper materials. Here, we report a method to prepare ultrastrong graphene fibers (GFs)-Cu core-shell wires with significantly enhanced electrical and mechanical properties. The core GFs are synthesized by chemical vapor deposition, followed by electroplating of Cu shells, where the large surface area of GFs in contact with Cu maximizes the mechanical toughness of the core-shell wires. At the same time, the unique electrical and thermal characteristics of graphene allow a ∼10 times higher current density limit, providing more efficient and reliable delivery of electrical energies through the GFs-Cu wires. We believe that our results would be useful to overcome the current limit in electrical wires and cables for lightweight, energy-saving, and high-power applications.