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Novel two-dimensional semiconductor crystals can exhibit diverse physical properties beyond their inherent semiconducting attributes, making their pursuit paramount. Memristive properties, as exemplars of these attributes, are predominantly manifested in wide-bandgap materials. However, simultaneously harnessing semiconductor properties alongside memristive characteristics to produce memtransistors is challenging. Herein we prepared a class of semiconducting III–V-derived van der Waals crystals, specifically the HxA1–xBX form, exhibiting memristive characteristics. To identify candidates for the material synthesis, we conducted a systematic high-throughput screening, leading us to 44 prospective III–V candidates; of these, we successfully synthesized ten, including nitrides, phosphides, arsenides and antimonides. These materials exhibited intriguing characteristics such as electrochemical polarization and memristive phenomena while retaining their semiconductive attributes. We demonstrated the gate-tunable synaptic and logic functions within single-gate memtransistors, capitalizing on the synergistic interplay between the semiconducting and memristive properties of our two-dimensional crystals. Our approach guides the discovery of van der Waals materials with unique properties from unconventional crystal symmetries.

Molybdenum disulfide (MoS2) is a promising candidate for next-generation transistor channel materials, boasting outstanding electrical properties and ultrathin structure. Conventional ion implantation processes are unsuitable for atomically thin two-dimensional (2D) materials, necessitating nondestructive doping methods. We proposed a novel approach: tunable n-type doping through sulfur vacancies (VS) and p-type doping by nitrogen substitution in MoS2, controlled by the duration of NH3plasma treatment. Our results reveal that NH3plasma exposure of 20 s increases the 2D sheet carrier density (n2D) in MoS2field-effect transistors (FETs) by +4.92 × 1011cm–2at a gate bias of 0 V, attributable to sulfur vacancy generation. Conversely, treatment of 40 s reduces n2Dby −3.71 × 1011cm–2due to increased nitrogen doping. X-ray photoelectron spectroscopy, Raman spectroscopy, and photoluminescence analyses corroborate these electrical characterization results, indicating successful n- and p-type doping. Temperature-dependent measurements show that the Schottky barrier height at the metal–semiconductor contact decreases by −31 meV under n-type conditions and increases by +37 meV for p-type doping. This study highlights NH3plasma treatment as a viable doping method for 2D materials in electronic and optoelectronic device engineering.

As semiconductor scaling continues to reach sub-nanometer levels, two-dimensional (2D) semiconductors are emerging as a promising candidate for the post-silicon material. Among these alternatives, Bi2O2Se has risen as an exceptionally promising 2D semiconductor thanks to its excellent electrical properties, attributed to its appropriate bandgap and small effective mass. However, unlike other 2D materials, growth of large-scale Bi2O2Se films with precise layer control is still challenging due to its large surface energy caused by relatively strong interlayer electrostatic interactions. Here, we present the successful growth of a wafer-scale (∼3 cm) Bi2O2Se film with precise thickness control down to the monolayer level on TiO2-terminated SrTiO3using metal–organic chemical vapor deposition (MOCVD). Scanning transmission electron microscopy (STEM) analysis confirmed the formation of a [BiTiO4]1–interfacial structure, and density functional theory (DFT) calculations revealed that the formation of [BiTiO4]1–significantly reduced the interfacial energy between Bi2O2Se and SrTiO3, thereby promoting 2D growth. Additionally, spectral responsivity measurements of two-terminal devices confirmed a bandgap increase of up to 1.9 eV in monolayer Bi2O2Se, which is consistent with our DFT calculations. Finally, we demonstrated high-performance Bi2O2Se field-effect transistor (FET) arrays, exhibiting an excellent average electron mobility of 56.29 cm2/(V·s). This process is anticipated to enable wafer-scale applications of 2D Bi2O2Se and facilitate exploration of intriguing physical phenomena in confined 2D systems.

Formation of charged trions is detrimental to the luminescence quantum efficiency of colloidal quantum dot (QD) thin films as they predominantly undergo nonradiative recombination. In this regard, control of charged trion formation is of interest for both fundamental characterization of the quasi-particles and performance optimization. Using CdSe/CdS QDs as a prototypical material system, here we demonstrate a metal-oxide-semiconductor capacitor based on QD thin films for studying the background charge effect on the luminescence efficiency and lifetime. The concentration ratio of the charged and neutral quasiparticles in the QDs is reversibly controlled by applying a gate voltage, while simultaneous steady-state and time-resolved photoluminescence measurements are performed. Notably, the photoluminescence intensity is modulated by up to 2 orders of magnitude with a corresponding change in the effective lifetime. In addition, chip-scale modulation of brightness is demonstrated, where the photoluminescence is effectively turned on and off by the gate, highlighting potential applications in voltage-controlled electrochromics.

This study demonstrates transparent and flexible capacitive pressure sensors using a high-kionic gel composed of an insulating polymer (poly(vinylidene fluoride-co-trifluoroethylene-co-chlorofluoroethylene), P(VDF-TrFE-CFE)) blended with an ionic liquid (IL; 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl) amide, [EMI][TFSA]). The thermal melt recrystallization of the P(VDF-TrFE-CFE):[EMI][TFSA] blend films develops the characteristic topological semicrystalline surface of the films, making them highly sensitive to pressure. Using optically transparent and mechanically flexible graphene electrodes, a novel pressure sensor is realized with the topological ionic gel. The sensor exhibits a sufficiently large air dielectric gap between graphene and the topological ionic gel, resulting in a large variation in capacitance before and after the application of various pressures owing to the pressure-sensitive reduction of the air gap. The developed graphene pressure sensor exhibits a high sensitivity of 10.14 kPa–1at 20 kPa, rapid response times of <30 ms, and durable device operation with 4000 repeated ON/OFF cycles. Furthermore, broad-range detections from lightweight objects to human motion are successfully achieved, demonstrating that the developed pressure sensor with a self-assembled crystalline topology is potentially suitable for a variety of cost-effective wearable applications.

Free-standing and film-type moisture-driven energy generators (MEGs) that harness the preferential interaction of ionized moisture with hydrophilic materials are interesting because of their wearability and portability without needing a water container. However, most such MEGs work in limited humidity conditions, which provide a substantial moisture gradient. Herein, we present a high-performance MEG with sustainable power-production capability in a wide range of environments. The bilayer-based device comprises a negatively surface-charged, hydrophilic MXene (Ti3C2Tx) aerogel and polyacrylamide (PAM) ionic hydrogel. The preferential selection on the MXene aerogel of positive charges supplied from the salts and water in the hydrogel is predicted by the first-principle simulation, which results in a high electric output in a wide relative humidity range from 20% to 95%. Furthermore, by replacing the hydrogel with an organohydrogel of PAM that has excellent water retention and structural stability, a device with long-term electricity generation is realized for more than 15 days in a broad temperature range (from −20 to 80 °C). Our MXene aerogel MEGs connected in series supply sufficient power for commercial electronic components in various outdoor environments. Moreover, an MXene aerogel MEG works as a self-powered sensor for recognizing finger bending and facial expression.

Wearable strain sensors have aroused increasing interest in human motion monitoring, even for the detection of small physiological signals such as joint movement and pulse. Stable monitoring of underwater human motion for a long time is still a notable challenge, as electronic devices can lose their effectiveness in a wet environment. In this study, a superhydrophobic and conductive knitted polyester fabric-based strain sensor was fabricated via dip coating of graphene oxide and polydimethylsiloxane micro/nanoparticles. The water contact angle of the obtained sample was 156°, which was retained above 150° under deformation (stretched to twice the original length or bent to 80°). Additionally, the sample exhibited satisfactory mechanical stability in terms of superhydrophobicity and conductivity after 300 abrasion cycles and 20 accelerated washing cycles. In terms of sensing performance, the strain sensor showed a rapid and obvious response to different deformations such as water vibration, underwater finger bending, and droplet shock. With the good combination of superhydrophobicity and conductivity, as well as the wearability and stretchability of the knitted polyester fabric, this wireless strain sensor connected with Bluetooth can allow for the remote monitoring of water sports, e.g., swimming, and can raise an alert under drowning conditions.

The development of electrodes with high conductivity, optical transparency, and reliable mechanical flexibility and stability is important for numerous solution-processed photoelectronic applications. Although transparent Ti3C2TXMXene electrodes with high conductivity are promising, their suitability for displays remains limited because of the high sheet resistance, which is caused by undesirable flake junctions and surface roughness. Herein, a flexible and transparent electrode has been fabricated that is suitable for a full-solution-processed quantum dot light-emitting diode (QLED). An MXene–silver nanowire (AgNW) hybrid electrode (MXAg) consists of a highly conductive AgNW network mixed with solution-processed MXene flakes. Efficient welding of wire-to-wire junctions with MXene flakes yields an electrode with a low sheet resistance and a high transparency of approximately 13.9 Ω sq–1and 83.8%, respectively. By employing a thin polymer buffer layer of poly(methyl methacrylate) (PMMA), followed by mild thermal treatment, a hybrid PMMA-based MXene–AgNW (MXAg@PMMA) electrode in which the work function of an MXAg hybrid FTE physically embedded in PMMA (MXAg@PMMA) can be tuned by controlling the amount of MXene in the hybrid film facilitates the development of a high-performance solution-processed QLED that exhibits maximum external quantum and current efficiencies of approximately 9.88% and 25.8 cd/A, respectively, with excellent bending stability. This work function-tunable flexible transparent electrode based on solution-processed nanoconductors provides a way to develop emerging high-performance, wearable, cost-effective, and soft electroluminescent devices.

Zn‐polyiodide redox flow battery is considered to be promising energy storage systems. However, the rate of the I3−(aq)/I−(aq) half redox reaction could be limited by a metastable iodine film in aqueous solutions. In this article, we found that the addition of Br−could inhibit the formation of an iodine film (I2‐F) and form soluble I2Br−(aq) during the electrooxidation of I−. I−was electrochemically oxidized to the soluble form I3−(aq). The depletion of I−(aq) and an increase of I3−(aq) would lead to the formation of I2and form I2‐F. Then, under a steady state, I−(aq) was electrochemically oxidized to I3−(aq) via I2‐F. However, the reaction pathway for the electrooxidation of I−was significantly altered by the addition of Br−. I−was electrochemically oxidized to I3−(aq) and was further oxidized to I2Br−(aq) without the formation of I2‐F. Moreover, we estimated the stability constant of I2Br−(aq) and consequently the fractional diagrams of I2(aq), I3−(aq), and I2Br−(aq) existing in a solution with both I−and Br−during the electrooxidation of I−, providing the necessity of a highly concentrated Br−condition in the vicinity of an electrode to form I2Br−(aq) as the main iodine species through the electrooxidation of I−. Zn‐polyiodide redox flow battery is considered to be promising energy storage systems. Nevertheless, the overall battery performance could suffer from the rate of the triiodide/iodide half redox reaction due to in situ formation of a metastable iodine film in aqueous solution. In this article, we present that the addition of bromide could inhibit the formation of an iodine film and form soluble iodine bromide anion during the electro‐oxidation of iodide.

The growth control of a molybdenum disulfide (MoS2) thin film, including the number of layers, growth rate, and electrical property modulation, remains a challenge. In this study, we synthesized MoS2thin films using the metal–organic chemical vapor deposition (MOCVD) method with a 2 inch wafer scale and achieved high thickness uniformity according to the positions on the substrate. In addition, we successfully controlled the number of MoS2layers to range from one to five, with a growth rate of 10 min per layer. The layer-dependent optical and electrical properties were characterized by photoluminescence, Raman spectroscopy, differential reflectance spectroscopy, and field effect transistors. To guide the growth of MoS2, we summarized the relation between the growth aspects and the precursor control in the form of a growth map. Reference to this growth map enabled control of the growth rate, domain density, and domain size according to the application purposes. Finally, we confirmed the electrical performance of MOCVD-grown MoS2with five layers under a high-κ dielectric environment, which exhibited an on/off current ratio of 10∼6and a maximum field effect mobility of 8.6 cm2V–1s–1.

Band engineering using the van der Waals heterostructure of two-dimensional materials allows for the realization of high-performance optoelectronic devices by providing an ultrathin and uniform PN junction with sharp band edges. In this study, a highly sensitive photodetector based on the van der Waals heterostructure of WSe2and MoS2was developed. The MoS2was utilized as the channel for a phototransistor, whereas the WSe2–MoS2PN junction in the out-of-plane orientation was utilized as a charge transfer layer. The vertical built-in electric field in the PN junction separated the photogenerated carriers, thus leading to a high photoconductive gain of 106. The proposed phototransistor exhibited an excellent performance, namely, a high photoresponsivity of 2700 A/W, specific detectivity of 5 × 1011Jones, and response time of 17 ms. The proposed scheme in conjunction with the large-area synthesis technology of two-dimensional materials contributes significantly to practical photodetector applications.

Lead halide perovskites have received much attention as light emitting materials owing to their excellent photoelectronic properties. Despite their high efficiency as light-emitting diodes (LEDs), only a few lead bromide perovskite (APbBr3)-based devices have been developed due to their low stabilities and/or the formation of undesirable phases under ambient condition. This work demonstrates that the addition of a small quantity of guanidinium (GUA) A-site cations into an all-inorganic CsPbBr3perovskite framework leads to the formation of multidimensional perovskites, with enhanced photoluminescence efficiency due to charge carrier funneling and a pinhole-free surface morphology. All-inorganic 3D CsPbBr3perovskite films and GUA-incorporated multidimensional quasi-2D films are employed in the fabrication of green LED devices with an inverted structure of glass substrate/indium tin oxide (ITO)/zinc oxide (ZnO)/poly(ethylenimine) (PEI)/perovskite/poly(9-vinylcarbazole) (PVK)/WO3/Al. With the addition of GUA A-site cations, the LEDs based on GUA-incorporated perovskite thin films exhibited much higher brightness of ∼10000 cd m–2and current efficiency of 9.4 cd A–1compared to those of Cs-only perovskite thin film LEDs (∼400 cd m–2and 0.2 Cd A–1, respectively).

Despite the great interest in inorganic halide perovskites (IHPs) for a variety of photoelectronic applications, environmentally robust nanopatterns of IHPs have hardly been developed mainly owing to the uncontrollable rapid crystallization or temperature and humidity sensitive polymorphs. Herein, we present a facile route for fabricating environment- and phase-stable IHP nanopatterns over large areas. Our method is based on nanoimprinting of a soft and moldable IHP adduct. A small amount of poly(ethylene oxide) was added to an IHP precursor solution to fabricate a spin-coated film that is soft and moldable in an amorphous adduct state. Subsequently, a topographically prepatterned elastomeric mold was used to nanoimprint the film to develop well-defined IHP nanopatterns of CsPbBr3and CsPbI3of 200 nm in width over a large area. To ensure environment- and phase-stable black CsPbI3nanopatterns, a polymer backfilling process was employed on a nanopatterned CsPbI3. The CsPbI3nanopatterns were overcoated with a thin poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE) film, followed by thermal melting of PVDF-TrFE, which formed the air-exposed CsPbI3nanopatterns laterally confined with PVDF-TrFE. Our polymer backfilled CsPbI3nanopatterns exhibited excellent environmental stability over one year at ambient conditions and for 10 h at 85 °C, allowing the development of arrays of two-terminal, parallel-type photodetectors with nanopatterned photoactive CsPbI3channels. Our polymer-assisted nanoimprinting offers a fast, low-pressure/temperature patterning method for high-quality nanopatterns on various substrates over a large area, overcoming conventional costly time-consuming lithographic techniques.

A triboelectric nanogenerator (TENG) is of tremendous interest owing to its high energy efficiency with a simple device architecture and applicability to various materials. Most previous topological surface modifications introduced for further improving the performance of a TENG are detrimental because they require expensive and/or harsh (e.g., high temperature and acidity) postetching processes, which limit the material choice and design of its components. Herein, we demonstrate an one-step route for developing rapid wet-processable surface-conformal triboelectric nanoporous films (STENFs). Our method is based on a simple supramolecular assembly of a ternary polymer blend suitable for various conventional solution processes such as spin-, bar-, spray-, and dip-coating. The one-step wet process of a ternary solution produces thin large-area films in which self-assembled, ordered nanopores of approximately 33 nm in diameter are developed even without an additional etching process. The study reveals that the small amount of amine-terminated poly(ethylene oxide) added to the binary blend of sulfonic-acid-terminated poly(styrene) and poly(2-vinylpyridine) efficiently activates the formation of spontaneous nanopores as a pore-generating agent. Our STENF significantly enhances the open-circuit voltage up to 1.5 times higher than that of a planar one, leading to an improved power density of approximately 77 μW/cm2. The suitability for diverse conventional coating processes offers a convenient approach for fabricating high-performance STENFs not only on flat substrates such as metals, polymers, and oxides but also on topological ones including wrinkled, roughened surfaces, textile fibers, natural leaves, and fabrics over a large area.

This work demonstrates a high-performance and hysteresis-free field-effect transistor based on two-dimensional (2D) semiconductors featuring a van der Waals heterostructure, MoS2channel, and GaS gate insulator. The transistor exhibits a subthreshold swing of 63 mV/dec, an on/off ratio over 106within a gate voltage of 0.4 V, and peak mobility of 83 cm2/(V s) at room temperature. The low-frequency noise characteristics were investigated and described by the Hooge mobility fluctuation model. The results suggest that the van der Waals heterostructure of 2D semiconductors can produce a high-performing interface without dangling bonds and defects caused by lattice mismatch. Furthermore, a logic inverter and a NAND gate are demonstrated, with an inverter voltage gain of 14.5, which is higher than previously reported by MoS2-based transistors with oxide dielectrics. Therefore, this transistor based on van der Waals heterostructure exhibits considerable potential in digital logic applications with low-power integrated circuits.

Plasmon resonance using metal nanostructures enables the realization of high-performance optoelectronic devices via field enhancements in the vicinity of the metal nanostructure. This study proposes an ultrabroadband MoS2photodetector based on the gap-mode plasmon of gold nanorods. The use of MoS2as a gap spacer for the gap-mode plasmon effect and as a channel material for the photodetector is demonstrated. The proposed photodetector demonstrates superior performance, a high photoresponsivity of 2.8 A/W at a near-infrared wavelength of 1100 nm, and a fast response time of 17 μs. In addition to the gap-mode plasmon effect of the gold nanorod enhancing the photoresponsivity from 1.13 to 8.7 A/W, the lateral surface plasmon resonance of the gold nanorods enhances the absorption of the longitudinal mode of the gold nanorods (near-infrared to infrared range). Further, the gap-mode plasmon effect of the gold nanorods enhances the absorption of the transverse mode of the gold nanorods (visible range), thus realizing ultrabroadband photodetection. Therefore, the proposed device design strategy contributes significantly to overcoming the trade-off between photoresponsivity and response time.

Simultaneous sensing and visualization of pressure provides a useful platform to obtain information about a pressurizing object, but the fabrication of such interactive displays at the single-device level remains challenging. Here, we present a pressure responsive electroluminescent (EL) display that allows for both sensing and visualization of pressure. Our device is based on a two-terminal capacitor with six constituent layers: top electrode/insulator/hole injection layer/emissive layer/electron transport layer/bottom electrode. Light emission upon exposure to an alternating current field between two electrodes is controlled by the capacitance change of the insulator arising from the pressure applied on top. Besides capacitive pressure sensing, our EL display allows for direct visualization of the static and dynamic information of position, shape, and size of a pressurizing object on a single-device platform. Monitoring the pressurized area of an elastomeric hemisphere on a device by EL enables quantitative estimation of the Young’s modulus of the elastomer, offering a new and facile characterization method for the mechanical properties of soft materials.

We demonstrated catechol lipid-based bioresin, which is collected from lacquer trees, to produce conductive pastes that can be processed at low temperatures, which are highly adhesive and multidurable. Our conductive paste, which consists of catechol lipid-based urushiol resin and a multimodal mixture of silver fillers, exhibited stable dispersion with shear thinning properties. The urushiol lacquer induced spontaneous reduction of silver salt at the surface of the silver fillers, thereby contributing to lower the contact resistance between conductive fillers in the electrical conduction. Furthermore, the directional volume shrinkage of the urushiol lacquer matrix in a cross-linking reaction resulted in a highly ordered microstructure of the silver fillers with layer-by-layer stacking of the silver flakes. This structure contributed to the improvement of the electrical contact between fillers as well as excellent mechanical hardness, anti-scratch capability, and the long-term environmental stability of the conductive films. Conductive films based on the silver paste with urushiol lacquer exhibited low electrical resistivity below 4.4 × 10–5Ω cm, 5B-class strong adhesion strength, and high hardness exceeding 200 MPa. Finally, we demonstrated the facile room-temperature processability and screen printability of the UL–Ag paste by fabricating a printed antenna and three-dimensional (3D) electrode assembly based on a plastic 3D block.

To achieve a highly realistic robot, closely mimicking human skin in terms of materials and functionality is essential. This paper presents an all-protein silk fibroin bionic skin (SFBS) that emulates both fast-adapting (FA) and slow-adapting (SA) receptors. The mechanically different silk film and hydrogel, which exhibited skin-like properties, such as stretchability (>140%), elasticity, low modulus (<10 kPa), biocompatibility, and degradability, were prepared through mesoscopic reconstruction engineering to mimic the epidermis and dermis. Our SFBS, incorporating SA and FA sensors, demonstrated a highly sensitive (1.083 kPa–1) static pressure sensing performance (in vitro and in vivo), showed the ability to sense high-frequency vibrations (50–400 Hz), could discriminate materials and sliding, and could even identify the fine morphological differences between objects. As proof of concept, an SFBS-integrated rehabilitation glove was synthesized, which could help stroke patients regain sensory feedback. In conclusion, this work provides a practical approach for developing skin equivalents, prostheses, and smart robots.

In the realm of energy harvesting, free-standing, film-type, moisture-driven electricity generators (MEGs) based on polymer hydrogels with moisture-retaining capability are promising as a convenient and practical power source, making them potentially suitable for various self-powered, wearable, and patchable electronic devices. Their performance is, however, substantially degraded under low-humidity (<40%) conditions owing to the limited water supply to the device. This study presents a high-performance film-type MEG that functions at a low humidity of 20%. The MEG is based on an ion-selective polymer aerogel as an electricity-generating layer, constructed on a water-collecting gel as a water reservoir. The water-collecting gel in the bi-layered MEG absorbs moisture even under low-humidity conditions and efficiently delivers moisture to the electricity-generating aerogel layer. The energy-harvesting ability of the electricity-generating aerogel layer is further facilitated by its characteristic vertical microstructure, which comprises aerogel pores directionally grown on the frozen water-collecting gel during the freeze-drying process. The low humidity-tolerant MEG generated a stable open-circuit voltage of 1.1V for more than 500min even under dry conditions (20% relative humidity). Various self-powered electronic applications are demonstrated with the low-humidity-tolerant, bi-layered MEGs in dry environments. This study provides new insights for designing future MEGs for operation in low-humidity environments, further facilitating the development of green and sustainable power generation.

The development of high-performance printable electrical circuits, particularly based on liquid metals, is fundamental for device interconnection in flexible electronics, motivating numerous attempts to develop a variety of alloys and their composites. Despite their great potential, rewritable and printable electronic circuits based on liquid metals are still manufactured on demand. In this study, we demonstrate liquid metal-based hydrogels suitable for rewritable, printable electrical circuits. Our liquid metal hydrogels are based on sedimentation-induced composites of eutectic gallium–indium (EGaIn) particles in poly(ethylene glycol) diacrylate (PEGDA). The EGaIn particles are vertically phase-segregated in the PEGDA. When a composite surface with high EGaIn content is gently scratched, the surface covering PEGDA is removed, followed by the rupture of the native oxide layers of the particles, and the exposed EGaIn becomes conductive. The subsequent water-driven swelling of PEGDA on the scratched surface completely erases the conductive circuit, causing the system to reset. Our friction-responsive liquid metal hydrogel exhibits writing–erasing endurance for 20 cycles, with a dramatic change in the electrical resistance from metal (∼1 Ω) to insulator (∼107Ω). By employing surface friction pen printing, we demonstrate mechanically flexible, rewritable, printable electrical conductors suitable for displays.

Prior to the advent of the next-generation heater for wearable/on-body electronic devices, various properties are required, including conductivity, transparency, mechanical reliability, and conformability. Expansion to two-dimensional (2D) structure of metallic nanowires based on network- and mesh-type geometries has been widely exploited for realizing these heaters. However, the routes led to many drawbacks such as the low-density cross-bar linking, self-aggregation of wire, and high junction resistance. Although 2D carbon nanomaterials such as graphene and reduced graphene oxide (rGO) have shown their potentials for the purpose, CVD-grown graphene with sufficiently high conductivity was limited due to its poor processability for large-area applications, while rGO fabricated with a complex reduction process involving the use of toxic chemicals suffered from a low electrical conductivity. In this study, we demonstrate a simple and robust process, utilizing electrostatic assembling of negatively charged MXene flakes on a positively treated surface of substrate, for fabricating a metal-like 2D MXene thin film heater (TFH). Our TFH showed a high optical property (>65%), low sheet resistance (215 Ω/sq), fast electrothermal response (within dozens of seconds) with an intrinsically high electrical conductivity, and mechanical flexibility (up to 180° bending). Its capability for forming a firm and stable ionic-type interface with a counterpart surface allows us to develop a shape-adaptable and patchable thread heater (TH) that can be shaped on diverse substrates even under harsh conditions of conventional sewing or weaving processes. This work suggests that our shape-adaptable MXene heaters are potentially suitable not only for wearable devices for local heating and defrosting but also for a variety of emerging applications of soft actuators and wearable/flexible healthcare monitoring and thermotherapy.

Visualization of human senses has been of great interest for developing an emerging interactive display that can artificially stimulate synesthesia with numerous unprecedented applications. Especially, visualization of various daily sound and music, which are much more complicated than human touch, in a form of flexible thin film devices can be a great challenge. We present flexible artificial synesthesia electronics that visualize continuous and complicated sounds. The electronic device is made of a thin composite film of a piezoelectric polymer for sound generation and inorganic electroluminescence (EL) microparticles for direct visualization of input sound signals. Field-induced EL of the microparticles in the device depends upon the source sound wave, making their EL synchronized with sound arising from the piezoelectric actuation. The flexible artificial synesthesia devices with sound-synchronized EL (FASSEL) showed extreme mechanical tolerance that can be repeatedly folded and crumpled with visible sound, allowing a variety of unexplored applications including synchronous sound-lightings and wearable, on-body sound-vision systems to facilitate emotional interaction of human being with sound in a human-friendly form.

Stretchable alternating-current electroluminescent (ACEL) devices are required due to their potential in wearable, biomedical, e-skin, robotic, lighting, and display applications; however, one of the main hurdles is to achieve uniform electroluminescence with an optimal combination of transparency, conductivity, and stretchability in electrodes. We therefore propose a fabrication scheme involving strategically combining two-dimensional graphene layers with a silver nanowire (Ag NW)-embedded PEDOT:PSS film. The developed hybrid electrode overcomes the limitations of commonly known metallic NWs and ionic conductor-based electrodes for ACEL applications. Furthermore, the potential of the hybrid electrode is realized in demonstrating large-area stretchable ACEL devices composed of an 8 × 8 passive array. The prototype ACEL passive array demonstrates efficient and uniform electroluminescence under high levels of mechanical deformation such as bending, rolling, twisting, and stretching.

Ionic thermoelectric supercapacitors (ITESCs) produce orders of magnitude higher voltages than those of conventional thermoelectrics (TEs) based on the thermo-diffusion of electrons/holes and are therefore attractive for converting low-grade heat into electricity. The stretchability and stability of the whole ITESC are important for wearable heat harvesting applications. Recent studies on ITESC have focused on stretchable ionic TE electrolytes with a giant Seebeck coefficient, but there are no reports of fully stretchable ITESCs for wearable heat harvesting devices due to the lack of stretchable electrodes and stretchable ionic TE electrolytes with stability. Herein, we present a fully stretchable ITESC composed of stable high-performance ionic thermoelectric elastomer (ITE) electrolyte and stretchable gold nanowire (AuNW) electrodes. The ITE shows excellent air stability (> 60 d) in comparison to hydrogel-based electrolytes that are susceptible to dehydration in ambient conditions. Furthermore, the ITE exhibits an apparent thermopower up to 38.9 mV K–1and ionic conductivity of 3.76 × 10–1mS cm–1, which both are maintained up to a tensile strain of 250%. Finally, a fully stretchable ITESC with AuNW electrodes is developed which can harvest energy from thermal gradients during deformations.

We propose a new approach to fluorine-containing, high-χ styrenic block copolymers (BCPs) via side-chain modification in one block. Polystyrene-b-poly(2,2,2-trifluoroethyl acrylate)s (PS-b-PTFEAs) were synthesized by high-conversion transesterification in acrylate units of polystyrene-b-poly(tert-butyl acrylate)s (PS-b-PtBAs) with the narrow dispersity being unchanged. A simple modification from PtBA into PTFEA block effectuates a remarkable increase in Flory–Huggins interaction parameter (χ) between the two blocks, which measures χ = 30.86/T+ 0.160, where T(K) is absolute temperature. The smallest half-pitch feature size of lamellae was evaluated to be 5 nm in 6.3 kg/mol PS-b-PTFEA. For versatility in thin film application, our results also offer a rapid perpendicular orientation of lamellar microdomains in PS-b-PTFEA films supported on a neutral homopolymer mat (cross-linked poly(4-trifluoromethylstyrene)), in which the lamellar spacing (L0) between the as-spun film and equilibrium bulk gets closer as the molecular weight of BCPs increases.

Two-dimensional (2D) nanosheets of transition metal dichalcogenides (TMDs) are of significant interest for potential photoelectronic applications. However, the fabrication of solution-processed arrays of mechanically flexible thin TMD films-based vertical type p–n junction photodetectors over a large area is a great challenge. Our method is based on controlled solvent evaporation of MoSe2suspension spread on water surface. Single or few-layered MoSe2nanosheets modified with the dispersant amine-terminated poly(styrene) (PS-NH2) were homogeneously deposited and stacked on water upon solvent evaporation, giving rise to uniform MoSe2/PS-NH2composite films that can be readily transferred onto other substrates. A p–n junction vertical diode of Al/p-type Si/p-type poly(9,9-di-n-octylfluorenyl-2,7-diyl)/n-type MoSe2composite/Au stacked from bottom to top exhibited characteristic rectifying current behavior upon voltage sweep with a rectification ratio of 103. Subsequent illumination of near-infrared light on the device resulted in a substantially enhanced dark current of approximately 103times greater than that of the nonexposed device. The photodetection performance, that is, switching time, responsivity, and detectivity, were 100.0 ms, 2.5 AW–1, and 2.34 × 1014, respectively. Furthermore, the performance of mechanically flexible photodetectors devices was comparable with that of the devices fabricated on the hard Si substrate even after 1000 bending cycles at a bending diameter of 7.2 mm.

Triboelectric nanogenerators (TENG) is of great interest as an emerging power harvester due to its simple device architecture and high efficiency. Despite development of various surface modification techniques for enhancing the performance of a TENG with a given triboelectric pair of materials, a method capable of being used universally on a variety of surfaces and improving the performance of TENGs with diverse surfaces remains a challenge. Here, we demonstrate a novel transfer-printing technique of hierarchically dewetted polymer droplets on various TENG surfaces for performance enhancement of the TENGs. Our method is based on controlled dewetting of a thin supramolecular assembled film of two end-functionalized polymer blends on a prepatterned poly(dimethyl siloxane) mold, followed by the physical pattern-transfer of arrays of the dewetted droplets consisting of supramolecular assembled nanostructures on a TENG contact surface. The hierarchically dewetted microdroplets comprising soft-etched nanopores efficiently improve the performance of a TENG by more than three times compared to one without the transferred pattern. The pattern-transfer is successfully achieved on various surfaces including not only oxides, plastics, rubbers, and metals, but also fabrics, coins, vegetables, and shells, making our approach a convenient way for enhancing the triboelectric performance of a given TENG.

Since the conventional fluorine-based electro-active polymers release toxic residues into the environment during their syntheses and decomposition processes, eco-friendly piezoelectric polymers are urgently demanded in the field of energy-related soft materials. Here, we derive a high-performance biodegradable chitin polymer from squid pen material and demonstrate its utility as a flexible piezoelectric material. The readily controlled ferroelectric chitin film confers excellent piezoelectricity under external mechanical pressure, resulting in comparable performance with that of conventional fluorine-based piezoelectric polymers. In particular, the sufficient piezoelectric behavior in chitin film allows us to not only realize a high-fidelity paper-type speaker and microphone that operates over a wide frequency range without significantly deteriorating the input and output sounds but also demonstrate transparent speaker consisting of AgNWs electrodes onto freestanding chitin film which also enables to resemble the original sound. Finally, the biodegradable chitin polymer can be successfully dissolved by chitinase enzyme within eight days without any toxic residues remained.

The development of electrically responsive sensors based on the capacitance, voltage, and resistance that can detect and simultaneou sly visualize the large strain involved with human motion is in great demand. Here, we demonstrate a highly stretchable, large strain capacitive sensor that can visualize strain based on the strain-responsive structural color (SC). Our device contains an elastomeric sensing film that produces a capacitance change under strain, in which a self-assembled block copolymer (BCP) photonic crystal (PC) film with 1D periodic in-plane lamellae aligned parallel to the film surface is embedded for the efficient visualization of strain. The capacitance change arises from changes in the dimensions of the elastomer film under strain. The mechanochromic BCP PC film responds to strain, giving rise to an SC change with strain. The initial red SC of the sensor blueshifts and turns blue when the sensor is stretched to 100%, resulting in a full-color SC alteration as a function of the strain. Our BCP SC strain sensor exhibits a fast strain response with multi-cycle reliability of both the capacitance and SC changes over 1000 cycles. This property allows for efficient visible recognition not only of the strained positions during finger bending and poking with a sharp object but also of the shapes of the strained objects. A strain sensor that changes color when stretched has been developed by a team in Korea. Flexible sensors that measure pressure or strain could find application as wearable health monitors. One route to achieve such sensors is to use dielectric films whose capacitance changes in response to mechanical stimulus. However, an easy way is needed for wearers to read the output. Cheolmin Park from Yonsei University and colleagues constructed a polymer-based material with a periodic structure that reflects light of different colors depending on the degree to which it is extended. Specifically, they created a block copolymer soft-solid film with one-dimensional periodic layers. The capacitance changes under strain as a result of the dimensional change of the elastomer film, causing the initially red sensor to turn blue when fully stretched. A novel block copolymer structural color strain sensor was developed, capable of electrically sensing a strain in capacitance change with simultaneous visualization of the strain. A thin mechanochromic bilayer of a block copolymer structural film with 1-D periodic lamellae placed on an ionic gel layer allowed for direct visualization of strain while sensing in capacitance when embedded in an elastomeric dielectric medium. Our block copolymer structural strain sensor was suitable for a reflective mode electronic skin which readily recognized human motion of the finger, elbow, and knee.

We report femtosecond infrared laser-induced selective tailoring of carrier transport as well as surface morphology on a conducting polymer blend thin film. Maximal 2.4 times enhancement on vertical current transport in poly(3-hexylthiophene):phenyl-C61-butyric acid methyl ester, was achieved by this irradiation. The laser irradiation induced a photo expansion without deteriorating its molecular structure and the film morphology could be customized in the micron scale by adjusting the laser writing parameters. In the photoexpanded region, the face-on populations were about 2.2 times larger in comparison with the pristine region, which was a major contributor to the enhanced carrier transport.

Sophisticated preparation of arbitrarily long conducting nanowire electrodes on a large area is a significant requirement for development of transparent nanoelectronics. We report a position-customizable and room-temperature-processable metallic nanowire (NW) electrode array using aligned NW templates and a demonstration of transparent all-NW-based electronic applications by simple direct-printing. Well-controlled electroless-plating chemistry on a polymer NW template provided a highly conducting Au NW array with a very low resistivity of 7.5 μΩ cm (only 3.4 times higher than that of bulk Au), high optical transmittance (>90%), and mechanical bending stability. This method enables fabrication of all-NW-based electronic devices on various nonplanar surfaces and flexible plastic substrates. Our approach facilitates realization of advanced future electronics.

Organic field effect transistor based nonvolatile memory (OFET-NVM) with semiconducting nanofloating gates offers additional benefits over OFET-NVMs with conventional metallic floating gates due to the facile controllability of charge storage based on the energetic structure of the floating gate. In particular, an all-in-one tunneling and floating-gate layer in which the semiconducting polymer nanodomains are self-assembled in the dielectric tunneling layer is promising. In this study, we utilize crystals of a p-type semiconducting polymer in which the crystalline lamellae of the polymer are spontaneously developed and embedded in the tunneling matrix as the nanofloating gate. The widths and lengths of the polymer nanodomains are approximately 20 nm and a few hundred nanometers, respectively. An OFET-NVM containing the crystalline nanofloating gates exhibits memory performance with a large memory window of 10 V, programming/erasing switching endurance for over 500 cycles, and a long retention time of 5000 s. Moreover, the device performance is improved by comixing with an n-type semiconductor; thus, the solution-processed p- and n-type double floating gates capable of storing both holes and electrons allow for the multilevel operation of our OFET-NVM. Four highly reliable levels (two bits per cell) of charge trapping and detrapping are achieved using this OFET-NVM by accurately choosing the programming/erasing voltages.

Inorganic perovskite nanocrystals (IPNCs) have attracted considerable attention due to their excellent optoelectronic properties. However, problems arise from anion migration during the preparation of a blue light-emitting diode (LED), and only small-scale syntheses have been conducted on a laboratory scale. By using only Br as the anion here, CsPbBr3was synthesized in the form of nanoplatelets to eliminate the effects of anion migration and to prepare an inorganic perovskite nanoplatelet (IPNPL) emitting blue light. In addition, the synthesis was performed under ambient conditions at room temperature, and the synthetic process was shortened to enable large-scale synthesis. We used a 1 L bottle for large-scale synthesis, and a photoluminescence quantum yield (PLQY) of 78% was observed at 460 nm. We fabricated LEDs by using IPNPLs, and we observed an electroluminescence peak at 461 nm. The developed synthetic method is expected to pave the way for commercialization of IPNCs and the next-generation display market.

To overcome the image deterioration caused by pixel miniaturization resulting from the high-resolution trend of CIS (CMOS image sensor) technology, a photodiode working with an enhanced mechanism based on a distinctive device structure from the existing one is considerably required. In this study, our photodiode, consisting of gold nanoparticles/monolayer graphene/n-type trilayer MoS2/p-type Si bulk, achieved ultrafast rising/falling times of 28.6 ns/30.4 ns due to the spatially confined narrow depletion width (DW) resulting from the 2D/3D heterojunction. To compensate for the expected low absorbance due to the narrow DW, plasmonic gold nanoparticles on monolayer graphene are introduced, revealing broadband enhanced EQE of an average of 187% in the spectral range of 420–730 nm and the maximum EQE reaching 847% at 5 nW for a 520 nm wavelength. The broadband enhancement was further investigated through multiphysics simulation, and carrier multiplication in graphene was discussed for the reason for exceeding 100% EQE in our reverse biased photodiode.

While tremendous efforts have been made for developing thin perovskite films suitable for a variety of potential photoelectric applications such as solar cells, field-effect transistors, and photodetectors, only a few works focus on the micropatterning of a perovskite film which is one of the most critical issues for large area and uniform microarrays of perovskite-based devices. Here we demonstrate a simple but robust method of micropatterning a thin perovskite film with controlled crystalline structure which guarantees to preserve its intrinsic photoelectric properties. A variety of micropatterns of a perovskite film are fabricated by either microimprinting or transfer-printing a thin spin-coated precursor film in soft-gel state with a topographically prepatterned elastomeric poly(dimethylsiloxane) (PDMS) mold, followed by thermal treatment for complete conversion of the precursor film to a perovskite one. The key materials development of our solvent-assisted gel printing is to prepare a thin precursor film with a high-boiling temperature solvent, dimethyl sulfoxide. The residual solvent in the precursor gel film makes the film moldable upon microprinting with a patterned PDMS mold, leading to various perovskite micropatterns in resolution of a few micrometers over a large area. Our nondestructive micropatterning process does not harm the intrinsic photoelectric properties of a perovskite film, which allows for realizing arrays of parallel-type photodetectors containing micropatterns of a perovskite film with reliable photoconduction performance. The facile transfer of a micropatterned soft-gel precursor film on other substrates including mechanically flexible plastics can further broaden its applications to flexible photoelectric systems.

One-dimensional photonic crystals based on the periodic stacking of two different dielectric layers have been widely studied, but the fabrication of mechanically flexible polymer structural color (SC) films, with electro-active color switching, remains challenging. Here, we demonstrate free-standing electric field tunable ionic liquid (IL) swollen block copolymer (BCP) films. Placement of a polymer/ionic liquid film-reservoir adjacent to a self-assembled poly(styrene-block-quaternized 2-vinylpyridine) (PS-b-QP2VP) copolymer SC film allowed the development of red (R), green (G), and blue (B) full-color SC block copolymer films by swelling of the QP2VP domains by the ionic liquid associated with water molecules. The IL–polymer/BCP SC film is mechanically flexible with excellent color stability over several days at ambient conditions. The selective swelling of the QP2VP domains could be controlled by both the ratio of the IL to a polymer in the gel-like IL reservoir layer and by an applied voltage in the range of −3 to +6 V using a metal/IL reservoir/SC film/IL reservoir/metal capacitor type device.

Design of materials to be heat-conductive in a preferred direction is a crucial issue for efficient heat dissipation in systems using stacked devices. Here, we demonstrate a facile route to fabricate polymer composites with directional thermal conduction. Our method is based on control of the orientation of fillers with anisotropic heat conduction. Melt-compression of solution-cast poly(vinylidene fluoride) (PVDF) and graphene nanoflake (GNF) films in an L-shape kinked tube yielded a lightweight polymer composite with the surface normal of GNF preferentially aligned perpendicular to the melt-flow direction, giving rise to a directional thermal conductivity of approximately 10 W/mK at 25 vol % with an anisotropic thermal conduction ratio greater than six. The high directional thermal conduction was attributed to the two-dimensional planar shape of GNFs readily adaptable to the molten polymer flow, compared with highly entangled carbon nanotubes and three-dimensional graphite fillers. Furthermore, our composite with its density of approximately 1.5 g/cm3was mechanically stable, and its thermal performance was successfully preserved above 100 °C even after multiple heating and cooling cycles. The results indicate that the methodology using an L-shape kinked tube is a new way to achieve polymer composites with highly anisotropic thermal conduction.

An understanding of the morphology-dependent correlation between photoluminescence and photoconductivity in nanostructured ZnO is important for elucidating the carrier dynamics and expanding its use in optoelectrical applications. In this study, we investigated this relationship using distinctly different ZnO nanorods with diameters greater than 100 nm, which were produced by a hydrothermal method. Furthermore, in order to study the effects of its defect states on the correlation, we thoroughly characterized the defect states of the ZnO nanorods in terms of the light-penetration depth during photoluminescence. The photoconductivities of the nanorods were measured using light sources with wavelengths of 355, 405, and 532 nm to confirm the influences of the visible-emission-generating defects on carrier transport. We found that the intensity of the near-band-edge emission was almost comparable to the amount of photocurrent generated under ultraviolet (UV) light; this could be attributed to the crystallinity of the inside of ZnO nanorods. However, the concentration of the surface defects resulting from the size and morphology probably had an effect, leading to the observed differences in the photocurrent sensitivity under low-intensity UV light, the dark current level, the amount of photocurrent under a specific wavelength of light within the visible range, and the persistent photoconductivity. The results of this study could aid research on carrier dynamics in nanostructured ZnO and further its use in optoelectronics.

The core components of a floating-gate organic thin-film transistor nonvolatile memory (OTFT-NVM) include the semiconducting channel layer, tunneling layer, floating-gate layer, and blocking layer, besides three terminal electrodes. In this study, we demonstrated OTFT-NVMs with all four constituent layers made of polymers based on consecutive spin-coating. Ambipolar charges injected and trapped in a polymer electret charge-controlling layer upon gate program and erase field successfully allowed for reliable bistable channel current levels at zero gate voltage. We have observed that the memory performance, in particular the reliability of a device, significantly depends upon the thickness of both blocking and tunneling layers, and with an optimized layer thickness and materials selection, our device exhibits a memory window of 15.4 V, on/off current ratio of 2 × 104, read and write endurance cycles over 100, and time-dependent data retention of 108s, even when fabricated on a mechanically flexible plastic substrate.

As one of the most emerging next-generation nonvolatile memories, one-transistor (1T)-type nonvolatile memories are of great attention due to their excellent memory performance and simple device architecture suitable for high density memory arrays. In particular, organic 1T-type memories containing both organic semiconductors and insulators are further beneficial because of their mechanical flexibility with low cost fabrication. Here, we demonstrate a new flexible organic 1T-type memory operating at low voltage. The low voltage operation of a memory less than 10 V was obtained by employing a polymer gate insulator solution blended with ionic liquid as a charge storage layer. Ionic liquid homogeneously dissolved in a thin poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE) film gave rise to low voltage operation of a device due to its high capacitance. Simultaneously, stable charge trapping of either anions or cations efficiently occurred in the polymer matrix, dependent upon gate bias. Optimization of ionic liquid in PVDF-TrFE thus led to an air-stable and mechanically flexible organic 1T-type nonvolatile memory operating at programming voltage of ±7 V with large ON/OFF current margin of approximately 103, reliable time-dependent data retention of more than 104seconds, and write/read endurance cycles of 80.

The authors investigated the microstructural and the electrical properties of ZnO, AZO, and SnO2based dye-sensitized solar cells (DSSCs) fabricated using a low-temperature-processed (200 °C) dye-sensitized ZnO, AZO, and SnO2nanoparticle thin film and a Pt catalyst deposited on ITO/glass by RF magnetron sputtering. A hydropolymer containing PEG (poly ethylene glycol) and PEO (poly ethylene oxide) is used to make uniformly-distributed ZnO, AZO, and SnO2nanoparticle layer which forms a nano porous ZnO, AZO, and SnO2network after heat treatment. The layer is then dye sensitized and sandwiched between two electrodes in an electrolyte to make a DSSC device. The highest measured parameters, the short-circuit current density (Jsc), the open circuit potential (Voc), the fill factor (FF), and power conversion efficiency (η), of the DSSC fabricated wander optimized conditions were observed to be 5.10 mA/cm2, 0.61 V, 0.46, and 1.43%, respectively.

Impressive biophotonic functions of flora in Mother Nature are often attributed to the optical diffraction occurring on hierarchically structured surfaces. The petals, displaying vivid colors, have diverse surface structures. The shapes of those structures alter significantly depending on the part of the petal, and they adjust the intensity of the reflected color and the light absorbance. Here, we added semiconducting properties to those intriguing optical functions arising from the unique surface structures. By means of atomic layer deposition (ALD), we conformally deposited a ZnO layer on the yellow rose petal, which has hierarchical surface structures and exhibits peculiar light absorbance behaviors. The resulting ZnO/petal composites revealed unique optoelectronic characteristics by synergetic effects between the biophotonic structures and inherent semiconducting properties. From several control experiments, we identified that the biophotonic hierarchical structures give rise to strong modulation of the light absorbance. We found that ZnO/petal exhibits superior mechanical stability to the raw petal likely due to the Zn infiltration into the petal. The design inspired by floral creatures with photonic structures and manufactured in the form of composite with mechanical stability and distinctive optoelectronic properties is believed to offer a new paradigm for the preparation of bioinspired photonic devices.

We present a simple but robust nondestructive process for fabricating micropatterns of thin ferroelectric polymer films with controlled crystals. Our method is based on utilization of localized heat arising from thin Ge8Sb2Te11(GST) alloy layer upon exposure of 650 nm laser. The heat was generated on GST layer within a few hundred of nanosecond exposure and subsequently transferred to a thin poly(vinylidene fluoride-co-trifluoroethylene) film deposited on GST layer. By controlling exposure time and power of the scanned laser, ferroelectric patterns of one or two microns in size are fabricated with various shape. In the micropatterned regions, ferroelectric polymer crystals were efficiently controlled in both degree of the crystallinity and the molecular orientations. Nonvolatile memory devices with laser scanned ferroelectric polymer layers exhibited excellent device performance of large remnant polarization, ON/OFF current ratio and data retention. The results are comparable with devices containing ferroelectric films thermally annealed at least for 2 h, making our process extremely efficient for saving time. Furthermore, our approach can be conveniently combined with a number of other functional organic materials for the future electronic applications.