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.

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.

Enhanced ultra high frequency EMI shielding with controlled ITO nano-branch width via different tin material types.

The development of technologies for electromagnetic wave contamination has garnered attention. Among the various electromagnetic wave frequencies, for high frequencies such as those in the K and Ka ranges, there is a limitation of using only the properties of a single material. Therefore, it is necessary to improve the absorption coefficients by increasing the path of electromagnetic waves through internal scattering at an interface or a structure inside the material. Here, we accurately demonstrated the role of Sn in the growth of an indium tin oxide (ITO) nano-branch structure and grew high-density ITO nano-branches with the lowest thickness possible. Consequently, we obtained shielding efficiencies of 21.09 dB (K band) and 17.81 dB (Ka band) for a film with a thickness of 0.00364 mm. Owing to the significantly high specific shielding efficiency and low thickness and weight, it is expected to be applied in various fields.

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.

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.

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.

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.

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.