Self-Healable Conductive Hydrogels with High Stretchability and Ultralow Hysteresis for Soft Electronics.

Stretchable sensors based on conductive hydrogels have attracted considerable attention for wearable electronics. However, their practical applications have been limited by the low sensitivity, high hysteresis, and long response times of the hydrogels. In this study, we developed high-performance poly(vinyl alcohol) (PVA)/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) based hydrogels post-treated with NaCl, which showed excellent mechanical properties, fast electrical response, and ultralow hysteresis properties. The hydrogels also demonstrated excellent self-healing properties with electrical and mechanical properties comparable to those of the original hydrogel and more than 150% elongation at break after the self-healing process. The high performance of the optimized hydrogels was attributed to the enhanced intermolecular forces between the PVA matrix and PEDOT:PSS, the favorable conformational change of the PEDOT chains, and an increase in localized charges in the hydrogel networks. The hydrogel sensors were capable of tracking large human motion and subtle muscle action in real time with high sensitivity, a fast response time (0.88 s), and low power consumption (<180 µW). Moreover, the sensor was able to monitor human respiration due to chemical changes in the hydrogel. These highly robust, stretchable, conductive, and self-healing PVA/PEDOT:PSS hydrogels, therefore, show great application potential as wearable sensors for monitoring human activity.

Universal Stretchable Conductive Cellulose/PEDOT:PSS Hybrid Films for Low Hysteresis Multifunctional Stretchable Electronics.

Skin-attachable conductive materials have attracted significant attention for use in wearable devices and physiological monitoring applications. Soft, skin-like conductive films must have excellent mechanical and electrical characteristics with on-skin conformability, stretchability, and robustness to detect body motion and biological signals. In this study, a conductive, stretchable, hydro-biodegradable, and highly robust cellulose/poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) hybrid film is fabricated. Through the synergetic interplay of a conductivity enhancer, nonionic fluorosurfactant, and surface modifier, the mechanical and electrical properties of the stretchable hybrid film are greatly improved. The stretchable cellulose/PEDOT:PSS hybrid film achieves a limited resistance change of only 1.21-fold after 100 stretch-release cycles (30% strain) with exceptionally low hysteresis, demonstrating its great potential as a stretchable electrode for stretchable electronics. In addition, the film shows excellent biodegradability, promising environmental friendliness, and safety benefits. High-performance stretchable cellulose/PEDOT:PSS hybrid films, which have high biocompatibility and sensitivity, are applied to human skin to serve as on-skin multifunctional sensors. The conformally mounted on-skin sensors are capable of continuously monitoring human physiological signals, such as body motions, drinking, respiration rates, vocalization, humidity, and temperature, with high sensitivity, fast responses, and low power consumption (21 µW). The highly conductive hybrid films developed in this study can be integrated as both stretchable electrodes and multifunctional healthcare monitoring sensors. We believe that the highly robust stretchable, conductive, biodegradable, skin-attachable cellulose/PEDOT:PSS hybrid films are worthy candidates as promising soft conductive materials for stretchable electronics.

Stretchable and Conductive Cellulose/Conductive Polymer Composite Films for On-Skin Strain Sensors.

Conductive composite materials have attracted considerable interest of researchers for application in stretchable sensors for wearable health monitoring. In this study, highly stretchable and conductive composite films based on carboxymethyl cellulose (CMC)-poly (3,4-ethylenedioxythiopehe):poly (styrenesulfonate) (PEDOT:PSS) (CMC-PEDOT:PSS) were fabricated. The composite films achieved excellent electrical and mechanical properties by optimizing the lab-synthesized PEDOT:PSS, dimethyl sulfoxide, and glycerol content in the CMC matrix. The optimized composite film exhibited a small increase of only 1.25-fold in relative resistance under 100% strain. The CMC-PEDOT:PSS composite film exhibited outstanding mechanical properties under cyclic tape attachment/detachment, bending, and stretching/releasing tests. The small changes in the relative resistance of the films under mechanical deformation indicated excellent electrical contacts between the conductive PEDOT:PSS in the CMC matrix, and strong bonding strength between CMC and PEDOT:PSS. We fabricated highly stretchable and conformable on-skin sensors based on conductive and stretchable CMC-PEDOT:PSS composite films, which can sensitively monitor subtle bio-signals and human motions such as respiratory humidity, drinking water, speaking, skin touching, skin wrinkling, and finger bending. Because of the outstanding electrical properties of the films, the on-skin sensors can operate with a low power consumption of only a few microwatts. Our approach paves the way for the realization of low-power-consumption stretchable electronics using highly stretchable CMC-PEDOT:PSS composite films.

Highly stretchable and robust transparent conductive polymer composites for multifunctional healthcare monitoring.

Soft, stretchable, conductive thin films have propelled to the forefront of applications in stretchable sensors for on-skin health monitoring. Stretchable conductive films require high conformability, stretchability, and mechanical/chemical stability when integrated into the skin. Here, we present a highly stretchable, conductive, and transparent natural rubber/silver nanowire (AgNW)/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) composite film. Overcoating the PEDOT:PSS layer results in outstanding mechanical robustness and chemical stability by suppressing the mechanical and chemical degradation of the nanowire networks. Moreover, the introduction of the organic surface modifier enhances the bonding strength between the natural rubber substrate and AgNW at the interface. The highly conformable composite films are integrated into multifunctional on-skin sensors for monitoring various human motions and biological signals with low-power consumption. We believe that the highly stretchable, robust, and conformable natural rubber/AgNW/PEDOT:PSS composite film can offer new opportunities for next-generation wearable sensors for body motion and physiological monitoring.

Effect of Laser-Induced Direct Micropatterning on Polymer Optoelectronic Devices.

Solution-processed polymer devices have been studied as a low-cost alternative to the conventional vacuum-processed organic devices. However, forming a specific pattern on polymer semiconductor films without costly lithography is still challenging. Herein, we report a low-cost direct patterning method for polymer optoelectronic devices, which can successfully engrave designated patterns on the polymer semiconductor layer regardless of its size and even after device encapsulation. Irradiation of a 100 ns pulse laser forms high-resolution patterns on devices such as polymer light-emitting diodes and polymer memory devices. The biggest advantage of the proposed patterning method is that it does not produce any physical damage in the device, such as leakage current or degraded light-emitting efficiency. Analysis confirms that the laser-induced heat alters the solid or crystal structure of the polymer semiconducting layers so that the designated areas of the polymer devices can be selectively and deliberately deactivated. We demonstrate the usability of the developed laser-induced direct-patterning method on the polymer devices by engraving a digital image onto "ON-state" light-emitting devices and by generating multiple states onto a 4 × 4 matrix polymer nonvolatile memory.

Simultaneously enhanced optical, electrical, and mechanical properties of highly stretchable transparent silver nanowire electrodes using organic surface modifier.

We report on a new surface modifier which simultaneously improves electrical, optical, and mechanical properties of silver nanowire-based stretchable transparent electrodes. The transparent electrodes treated with 11-aminoundecanoic acid achieve a low sheet resistance of 26.0 ohm/sq and a high transmittance of 90% with an excellent stretchability. These improvements are attributed to the effective formation of a strong chemical bond between silver nanowire networks and elastomeric substrates by 11-aminoundecanoic acid treatment. The resistance change of the optimized silver nanowire/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thin-films is only about 10% when the film is stretched by 120%. In addition, the chemical stability of stretchable silver nanowire films is significantly improved by the introduction of conductive PEDOT:PSS overcoat film. The optimized electrodes are utilized as high-performance stretchable transparent heaters, successfully illustrating its feasibility for future wearable electronics.

Enhanced outcoupling in down-conversion white organic light-emitting diodes using imprinted microlens array films with breath figure patterns.

We demonstrate high-performance down-conversion microlens array (DC-MLA) films for white organic light-emitting diodes (OLEDs). The DC-MLA films are readily fabricated by an imprinting method based on breath figure patterns, which are directly formed on the polymer substrate with a novel concept. The DC-MLA films result in high-quality white light as well as enhanced light outcoupling efficiency for white OLEDs. The external quantum efficiency and power efficiency of OLEDs with DC-MLA films are increased by a factor of 1.35 and 1.86, respectively, compared to OLEDs without outcoupling films. Moreover, the white OLEDs with DC-MLA films achieve a high color-rendering index of 84.3. It is anticipated that the novel DC-MLA films fabricated by the simple imprinting process with breath figure patterns can contribute to the development of efficient white OLEDs.

The role of cation and anion dopant incorporated into a ZnO electron transporting layer for polymer bulk heterojunction solar cells.

Doping is a widely-implemented strategy for enhancing the inherent electronic properties of charge transport layers in photovoltaic devices. A facile solution-processed zinc oxide (ZnO) and various cation and anion-doped ZnO layers were synthesized via the sol-gel method and employed as electron transport layers (ETLs) for inverted polymer solar cells (PSCs). The results indicated that all PSCs with doped ZnO ETLs exhibited better photovoltaic performance compared with the PSCs with a pristine ZnO ETL. By exploring the role of various anion and cation dopants (three compounds with the same Al3+ cation: Al(acac)3, Al(NO3)3, AlCl3 and three compounds with the same Cl- anion: NH4Cl, MgCl2, AlCl3), we found that the work function changed to favor electronic extraction only when the Cl anion was involved. In addition, the conductivity of ZnO was enhanced more with the Al3+ cation. Therefore, in inverted solar cells, doping with Al3+ and Cl- delivered the best power conversion efficiency (PCE). The maximum PCE of 10.38% was achieved from the device with ZnO doped with Al+ and Cl-.

Highly Enhanced Light-Outcoupling Efficiency in ITO-Free Organic Light-Emitting Diodes Using Surface Nanostructure Embedded High-Refractive Index Polymers.

We develop the high-performance internal light-outcoupling (HRLOC) system based on the high-refractive index polyimide (PI) and metal oxide nanoparticles for organic light-emitting diodes (OLEDs) with silver nanowires (AgNWs). The spontaneously formed nanobump structures, high refractive index, and light-scattering properties of HRLOC significantly enhance the light-extraction efficiency of OLEDs. Not only do the outcoupling structures improve the light-extraction efficiency, but also remarkably enhance the electrical properties of OLEDs. HRLOC leads to the regular and smooth formation of AgNWs, resulting in the improvement of the electrical properties of devices by preventing electrical shorts and leakage currents. The power efficiency of the AgNW-based OLEDs with PI is improved by a factor of 1.31 compared to the reference device with indium tin oxide (ITO) transparent electrode at a luminance of 20 000 cd/m2. The efficiency is further improved by incorporating TiO2 nanoparticles into the PI matrix by a factor of 1.69. To our knowledge, the optically and electrically enhanced OLEDs show one of the highest enhancement factors reported for ITO-free OLEDs with internal outcoupling structures. In addition, the outcoupling structures are solution processable, thermally stable, and can be scaled up to 200 × 200 mm2 for large-area applications. We believe that the light-outcoupling structures developed here have great potential for efficient, low-cost, and flexible ITO-free OLEDs.

Highly Conductive PEDOT:PSS Films with 1,3-Dimethyl-2-Imidazolidinone as Transparent Electrodes for Organic Light-Emitting Diodes.

Highly conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) ( PEDOT: PSS) films as transparent electrodes for organic light-emitting diodes (OLEDs) are doped with a new solvent 1,3-dimethyl-2-imidazolidinone (DMI) and are optimized using solvent post-treatment. The DMI doped PEDOT: PSS films show significantly enhanced conductivities up to 812.1 S cm(-1) . The sheet resistance of the PEDOT: PSS films doped with DMI is further reduced by various solvent post-treatment. The effect of solvent post-treatment on DMI doped PEDOT: PSS films is investigated and is shown to reduce insulating PSS in the conductive films. The solvent posttreated PEDOT: PSS films are successfully employed as transparent electrodes in white OLEDs. It is shown that the efficiency of OLEDs with the optimized DMI doped PEDOT: PSS films is higher than that of reference OLEDs doped with a conventional solvent (ethylene glycol). The results present that the optimized PEDOT: PSS films with the new solvent of DMI can be a promising transparent electrode for low-cost, efficient ITO-free white OLEDs.