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.

Monolithic Integration of Semi-Transparent and Flexible Integrated Image Sensor Array with a-IGZO Thin-Film Transistors (TFTs) and p-i-n Hydrogenated Amorphous Silicon Photodiodes.

A novel approach to fabricating a transparent and flexible one-transistor-one-diode (1T-1D) image sensor array on a flexible colorless polyimide (CPI) film substrate is successfully demonstrated with laser lift-off (LLO) techniques. Leveraging transparent indium tin oxide (ITO) electrodes and amorphous indium gallium zinc oxide (a-IGZO) channel-based thin-film transistor (TFT) backplanes, vertically stacked p-i-n hydrogenated amorphous silicon (a-Si:H) photodiodes (PDs) utilizing a low-temperature (<90 °C) deposition process are integrated with a densely packed 14 × 14 pixel array. The low-temperature-processed a-Si:H photodiodes show reasonable performance with responsivity and detectivity for 31.43 mA/W and 3.0 × 1010 Jones (biased at -1 V) at a wavelength of 470 nm, respectively. The good mechanical durability and robustness of the flexible image sensor arrays enable them to be attached to a curved surface with bending radii of 20, 15, 10, and 5 mm and 1000 bending cycles, respectively. These studies show the significant promise of utilizing highly flexible and rollable active-matrix technology for the purpose of dynamically sensing optical signals in spatial applications.

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.

Optimized Substrate Orientations for Highly Uniform Metal Halide Perovskite Film Deposition.

Uniform optoelectronic quality of metal halide perovskite (MHP) films is critical for scalable production in large-area applications, such as photovoltaics and displays. While vapor-based MHP film deposition is advantageous for this purpose, achieving film uniformity can be challenging due to uneven temperature distribution and precursor concentration over the substrate. Here, we propose optimized substrate orientations for the vapor-based fabrication of homogeneous MAPbI3 thin films, involving a PbI2 primary layer deposition and subsequent conversion using vaporized methylammonium iodide (MAI). Leveraging computational fluid dynamics (CFD) simulations, we confirm that vertical positioning during the PbI2 layer growth yields a uniform film with a narrow temperature distribution and minimal boundary layer thickness. However, during the subsequent conversion step, horizontal substrate positioning results in spatially more uniform MAPbI3 thickness and grain size compared to the vertical placement due to enhanced MAI intercalation. From this optimized substrate positioning, we observe substantial optical homogeneity across the substrate on a centimeter scale, along with uniform and enhanced optoelectronic device performance within photodetector arrays. Our results offer a potential path toward the scalable production of highly uniform perovskite films.

Direct Printing of Ultrathin Block Copolymer Film with Nano-in-Micro Pattern Structures.

Nanotransfer printing (nTP) is one of the most promising nanopatterning methods given that it can be used to produce nano-to-micro patterns effectively with functionalities for electronic device applications. However, the nTP process is hindered by several critical obstacles, such as sub-20 nm mold technology, reliable large-area replication, and uniform transfer-printing of functional materials. Here, for the first time, a dual nanopatterning process is demonstrated that creates periodic sub-20 nm structures on the eight-inch wafer by the transfer-printing of patterned ultra-thin (<50 nm) block copolymer (BCP) film onto desired substrates. This study shows how to transfer self-assembled BCP patterns from the Si mold onto rigid and/or flexible substrates through a nanopatterning method of thermally assisted nTP (T-nTP) and directed self-assembly (DSA) of Si-containing BCPs. In particular, the successful microscale patternization of well-ordered sub-20 nm SiOx patterns is systematically presented by controlling the self-assembly conditions of BCP and printing temperature. In addition, various complex pattern geometries of nano-in-micro structures are displayed over a large patterning area by T-nTP, such as angular line, wave line, ring, dot-in-hole, and dot-in-honeycomb structures. This advanced BCP-replicated nanopatterning technology is expected to be widely applicable to nanofabrication of nano-to-micro electronic devices with complex circuits.

Effect of Measurement System Configuration and Operating Conditions on 2D Material-Based Gas Sensor Sensitivity.

Gas sensors applied in real-time detection of toxic gas leakage, air pollution, and respiration patterns require a reliable test platform to evaluate their characteristics, such as sensitivity and detection limits. However, securing reliable characteristics of a gas sensor is difficult, owing to the structural difference between the gas sensor measurement platform and the difference in measurement methods. This study investigates the effect of measurement conditions and system configurations on the sensitivity of two-dimensional (2D) material-based gas sensors. Herein, we developed a testbed to evaluate the response characteristics of MoS2-based gas sensors under a NO2 gas flow, which allows variations in their system configurations. Additionally, we demonstrated that the distance between the gas inlet and the sensor and gas inlet orientation influences the sensor performance. As the distance to the 2D gas sensor surface decreased from 4 to 2 mm, the sensitivity of the sensor improved to 9.20%. Furthermore, when the gas inlet orientation was perpendicular to the gas sensor surface, the sensitivity of the sensor was the maximum (4.29%). To attain the optimum operating conditions of the MoS2-based gas sensor, the effects of measurement conditions, such as gas concentration and temperature, on the sensitivity of the gas sensor were investigated.

Robust 2D MoS2 Artificial Synapse Device Based on a Lithium Silicate Solid Electrolyte for High-Precision Analogue Neuromorphic Computing.

High-precision artificial synaptic devices compatible with existing CMOS technology are essential for realizing robust neuromorphic hardware systems with reliable parallel analogue computation beyond the von Neumann serial digital computing architecture. However, critical issues related to reliability and variability, such as nonlinearity and asymmetric weight updates, have been great challenges in the implementation of artificial synaptic devices in practical neuromorphic hardware systems. Herein, a robust three-terminal two-dimensional (2D) MoS2 artificial synaptic device combined with a lithium silicate (LSO) solid-state electrolyte thin film is proposed. The rationally designed synaptic device exhibits excellent linearity and symmetry upon electrical potentiation and depression, benefiting from the reversible intercalation of Li ions into the MoS2 channel. In particular, extremely low cycle-to-cycle variations (3.01%) during long-term potentiation and depression processes over 500 pulses are achieved, causing statistical analogue discrete states. Thus, a high classification accuracy of 96.77% (close to the software baseline of 98%) is demonstrated in the Modified National Institute of Standards and Technology (MNIST) simulations. These results provide a future perspective for robust synaptic device architecture of lithium solid-state electrolytes stacked with 2D van der Waals layered channels for high-precision analogue neuromorphic computing systems.

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.

Large emergent optoelectronic enhancement in molecularly cross-linked gold nanoparticle nanosheets.

A central goal in molecular electronics and optoelectronics is to translate tailorable molecular properties to larger materials and to the device level. Here, we present a method to fabricate molecularly cross-linked, self-assembled 2D nanoparticle sheets (X-NS). Our method extends a Langmuir approach of self-assembling gold nanoparticle (NP) arrays at an air-water interface by replacing the liquid sub-phase to an organic solvent to enable cross-linking with organic molecules, and then draining the sub-phase to deposit films. Remarkably, X-NS comprising conjugated oligophenylene dithiol cross-linkers (HS-(C6H4)n-SH, 1 ≤ n ≤ 3) exhibit increasing conductance with molecule length, ~6 orders of magnitude enhancement in UV-Vis extinction coefficients, and photoconductivity with molecule vs. NP contributions varying depending on the excitation wavelength. Finite difference time domain (FDTD) analyses and control measurements indicate that these effects can be modeled provided the local complex dielectric constant is strongly modified upon cross-linking. This suggests quantum hybridization at a molecule-band (q-MB) level. Given the vast number of molecules and nano-building blocks available, X-NS have potential to significantly increase the range of available 2D nanosheets and associated quantum properties.

Transparent and Flexible Electromagnetic Interference Shielding Film Using ITO Nanobranches by Internal Scattering.

A transparent and flexible film capable of shielding electromagnetic waves over a wide range of frequencies (X and Ku bands, 8-18 GHz) is prepared. The electromagnetic wave shielding film is fabricated using the excellent transmittance, electrical conductivity, and thermal stability of indium tin oxide (ITO), a representative transparent conductive oxide. The inherent mechanical brittleness of oxide ceramics is overcome by adopting a nanobranched structure. In addition, mechanical stability is maintained even after repeated bending experiments (200 000 times). The produced transparent and flexible shielding film is applied to practical GHz devices (Wi-Fi and LTE devices), and signal sensitivity is confirmed to decrease. Therefore, it can be widely applied to various transparent and flexible electronic devices.

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.

Stretchable Inorganic GaN-Nanowire Photosensor with High Photocurrent and Photoresponsivity.

To effectively implement wearable systems, their constituent components should be made stretchable. We successfully fabricated highly efficient stretchable photosensors made of inorganic GaN nanowires (NWs) as light-absorbing media and graphene as a carrier channel on polyurethane substrates using the pre-strain method. When a GaN-NW photosensor was stretched at a strain level of 50%, the photocurrent was measured to be 0.91 mA, corresponding to 87.5% of that (1.04 mA) obtained in the released state, and the photoresponsivity was calculated to be 11.38 A/W. These photosensors showed photocurrent and photoresponsivity levels much higher than those previously reported for any stretchable semiconductor-containing photosensor. To explain the superior performances of the stretchable GaN-NW photosensor, it was approximated as an equivalent circuit with resistances and capacitances, and in this way, we analyzed the behavior of the photogenerated carriers, particularly at the NW-graphene interface. In addition, the buckling phenomenon typically observed in organic-based stretchable devices fabricated using the pre-strain method was not observed in our photosensors. After a 1000-cycle stretching test with a strain level of 50%, the photocurrent and photoresponsivity of the GaN-NW photosensor were measured to be 0.96 mA and 11.96 A/W, respectively, comparable to those measured before the stretching test. To evaluate the potential of our stretchable devices in practical applications, the GaN-NW photosensors were attached to the proximal interphalangeal joint of the index finger and to the back of the wrist. Photocurrents of these photosensors were monitored during movements made about these joints.

Foldable Perovskite Solar Cells Using Carbon Nanotube-Embedded Ultrathin Polyimide Conductor.

Recently, foldable electronics technology has become the focus of both academic and industrial research. The foldable device technology is distinct from flexible technology, as foldable devices have to withstand severe mechanical stresses such as those caused by an extremely small bending radius of 0.5 mm. To realize foldable devices, transparent conductors must exhibit outstanding mechanical resilience, for which they must be micrometer-thin, and the conducting material must be embedded into a substrate. Here, single-walled carbon nanotubes (CNTs)-polyimide (PI) composite film with a thickness of 7 µm is synthesized and used as a foldable transparent conductor in perovskite solar cells (PSCs). During the high-temperature curing of the CNTs-embedded PI conductor, the CNTs are stably and strongly p-doped using MoO x , resulting in enhanced conductivity and hole transportability. The ultrathin foldable transparent conductor exhibits a sheet resistance of 82 Ω sq.-1 and transmittance of 80% at 700 nm, with a maximum-power-point-tracking-output of 15.2% when made into a foldable solar cell. The foldable solar cells can withstand more than 10 000 folding cycles with a folding radius of 0.5 mm. Such mechanically resilient PSCs are unprecedented; further, they exhibit the best performance among the carbon-nanotube-transparent-electrode-based flexible solar cells.

In Situ Vapor-Phase Halide Exchange of Patterned Perovskite Thin Films.

Metal halide perovskites (MHPs) exhibit optoelectronic properties that are dependent on their ionic composition, and the feasible exploitation of these properties for device applications requires the ability to control the ionic composition integrated with the patterning process. Herein, the halide exchange process of MHP thin films directly combined with the patterning process via a vapor transport method is demonstrated. Specifically, the patterned arrays of CH3 NH3 PbBr3 (MAPbBr3 ) are obtained by stepwise conversion from polymer-templated PbI2 thin films to CH3 NH3 PbI3 (MAPbI3 ), followed by halide exchange via precursor switching from CH3 NH3 I to CH3 NH3 Br. It is confirmed that the phase transformation from MAPbI3 patterns to MAPbBr3 shows time- and position-dependences on the substrate during halide exchange following the solid-solution model with Avrami kinetics. The photodetectors fabricated from the completely exchanged MAPbBr3 patterns display exceptional air stability and reversible detectivity from "apparent death" upon removing the adsorbed impurities, thereby suggesting the superior structural stability of perovskite patterns prepared through vapor-phase halide exchange. The results demonstrate the potential of chemical vapor deposition patterning of MHP materials in multicomponent optoelectronic device systems.

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.

Highly Efficient Photoelectrochemical Water Splitting Using GaN-Nanowire Photoanode with Tungsten Sulfides.

In the present study, we have achieved high-performance photoelectrochemical water splitting (PEC-WS) using GaN nanowires (NWs) coated with tungsten sulfide (WxS1-x) (GaN-NW-WxS1-x) as a photoanode. The measured current density and applied-bias photon-to-current efficiency were 20.38 mA/cm2 and 13.76%, respectively. These values were much higher than those reported previously for photoanodes with any kind of III-nitride nanostructure. The amount of hydrogen gas formed was 1.01 mmol/cm2 from 7 h PEC-WS, which was also much higher than the previously reported values. The drastic improvement in the PEC-WS performance using the GaN-NW-WxS1-x photoanode was attributed to an increase in the number of photogenerated carriers due to the highly crystalline GaN NWs, and acceleration of separation of photogenerated carriers and consequent suppression of charge recombination because of nitrogen-terminated surfaces of NWs, sulfur vacancies in WxS1-x, and type-II band alignment between NW and WxS1-x. The degree of impedance matching, evaluated from Nyquist plots, was considered to analyze charge transfer characteristics at the interface between the GaN-NW-WxS1-x photoanode and 0.5-M H2SO4 electrolyte. Considering the material system and scheme for the PEC-WS, our approach provides an efficient way to improve hydrogen evolution reaction.

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.