Ice-Templated,Large-Area Silver Nanowire Pattern for Flexible Transparent Electrode

Flexible transparent electrodes are critically important for the emerging flexible and stretchable electronic and optoelectronic devices. To this end, transparent polymer films coated with silver nanowires (AgNWs) have been intensively studied in the past decade. However, it remains a grand challenge to achieve both high conductivity and transmittance in large-area films, mainly due to the poor alignment of AgNWs and their high junction resistance. Here, the successful attempt to realize large-area AgNW patterns on various substrates by a 2D ice-templating approach is reported. With a relatively low dosage of AgNWs (4 µg·cm⁻²), the resulted flexible electrode simultaneously achieves high optical transmittance (≈91%) and low sheet resistance (20 Ω·sq⁻¹). In addition, the electrode exhibits excellent durability during cyclic bending (≈10 000 times) and stretching (50% strain). The potential applications of the flexible transparent electrode in both touch screen and electronic skin sensor, which can monitor the sliding pressure and direction in real-time, are demonstrated. More importantly, it is believed that the study represents a facile and low-cost approach to assemble various nanomaterials into large-area functional patterns for advanced flexible devices.     

Highly Conductive and Transparent PEDOT:PSS Films with a Fluorosurfactant for Stretchable and Flexible Transparent Electrodes

Highly conductive and transparent poly‐(3,4‐ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) films, incorporating a fluorosurfactant as an additive, have been prepared for stretchable and transparent electrodes. The fluorosurfactant‐treated PEDOT:PSS films show a 35% improvement in sheet resistance (R_s) compared to untreated films. In addition, the fluorosurfactant renders PEDOT:PSS solutions amenable for deposition on hydrophobic surfaces, including pre‐deposited, annealed films of PEDOT:PSS (enabling the deposition of thick, highly conductive, multilayer films) and stretchable poly(dimethylsiloxane) (PDMS) substrates (enabling stretchable electronics). Four‐layer PEDOT:PSS films have an R_s of 46 Ω per square with 82% transmittance (at 550 nm). These films, deposited on a pre‐strained PDMS substrate and buckled, are shown to be reversibly stretchable, with no change to R_s, during the course of over 5000 cycles of 0 to 10% strain. Using the multilayer PEDOT:PSS films as anodes, indium tin oxide (ITO)‐free organic photovoltaics are prepared and shown to have power conversion efficiencies comparable to that of devices with ITO as the anode. These results show that these highly conductive PEDOT:PSS films can not only be used as transparent electrodes in novel devices (where ITO cannot be used), such as stretchable OPVs, but also have the potential to replace ITO in conventional devices.     

Stretchable and Transparent Conductive PEDOT:PSS‐Based Electrodes for Organic Photovoltaics and Strain Sensors Applications

The development of transparent, conducting, and stretchable poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)‐based electrodes using a combination of a polyethylene oxide (PEO) polymer network and the surfactant Zonyl is reported. The latter improves the ductility of PEDOT:PSS and enables its deposition on hydrophobic surfaces such as polydimethylsiloxane (PDMS) elastomers, while the presence of a 3D matrix offers high electrical conductivity, elasticity, and mechanical recoverability. The resulting electrode exhibits attractive properties such as high electrical conductivity of up to 1230 S cm^?1 while maintaining high transparency of 95% at 550 nm. The potential of the electrode technology is demonstrated in indium‐tin‐oxide (ITO)‐free solar cells using the PBDB‐T‐2F:IT‐4F blend with a power conversion efficiency of 12.5%. The impact of repeated stretch‐and‐release cycles on the electrical resistance is also examined in the effort to evaluate the properties of the electrodes. The interpenetrated morphology of the PEDOT:PSS and polyethylene oxide network is found to exhibit beneficial synergetic effects resulting in excellent mechanical stretchability and high electrical conductivity. By carefully tuning the amount of additives, the ability to detect small changes in electrical resistance as a function of mechanical deformation is demonstrated, which enables the demonstration of stretchable and resilient on‐skin strain sensors capable of detecting small motions of the finger.     

Uniformly Interconnected Silver‐Nanowire Networks for Transparent Film Heaters

The fabrication and design principles for using silver‐nanowire (AgNW) networks as transparent electrodes for flexible film heaters are described. For best practice, AgNWs are synthesized with a small diameter and network structures of the AgNW films are optimized, demonstrating a favorably low surface resistivity in transparent layouts with a high figure‐of‐merit value. To explore their potential in transparent electrodes, a transparent film heater is constructed based on uniformly interconnected AgNW networks, which yields an effective and rapid heating of the film at low input voltages. In addition, the AgNW‐based film heater is capable of accommodating a large amount of compressive or tensile strains in a completely reversible fashion, thereby yielding an excellent mechanical flexibility. The AgNW networks demonstrated here possess attractive features for both conventional and emerging applications of transparent flexible electrodes.     

A Sensing and Stretchable Polymer-Dispersed Liquid Crystal Device Based on Spiderweb-Inspired Silver Nanowires-Micromesh Transparent Electrode

Polymer-dispersed liquid crystal (PDLC) devices are truly promising optical modulators for information display, smart window as well as intelligent photoelectronic applications due to their fast switching, large optical modulation as well as cost-effectiveness. However, realizing highly soft PDLC devices with sensing function remains a grand challenge because of the intrinsic brittleness of traditional transparent conductive electrodes. Here, inspired by spiderweb configuration, a novel type of silver nanowires (AgNWs) micromesh-based stretchable transparent conductive electrodes (STCEs) is developed to support the realization of soft PDLC device. Benefiting from the embedding design of AgNWs micromesh in polydimethylsiloxane (PDMS), the STCEs can maintain excellent electrical conductivity and transparency even in various extreme conditions such as bending, folding, twisting, stretching as well as multiple chemical corrosion. Further, STCEs with the embedded AgNWs micromesh endow the assembled PDLC device with excellent photoelectrical properties including rapid switching speed (<1 s), large optical modulation (69% at 600 nm), as well as robust mechanical stability (bending over 1000 cycles and stretching to 40%). Moreover, the device displays the pressure sensing function with high sensitivity in response to pressure stimulus. It is conceivable that AgNWs micromesh transparent electrodes will shape the next generation of related soft smart electronics.     

An Indium‐Free Anode for Large‐Area Flexible OLEDs: Defect‐Free Transparent Conductive Zinc Tin Oxide

Flexible large‐area organic light‐emitting diodes (OLEDs) require highly conductive and transparent anodes for efficient and uniform light emission. Tin‐doped indium oxide (ITO) is the standard anode in industry. However, due to the scarcity of indium, alternative anodes that eliminate its use are highly desired. Here an indium‐free anode is developed by a combinatorial study of zinc oxide (ZnO) and tin oxide (SnO₂), both composed of earth‐abundant elements. The optimized Zn–Sn–O (ZTO) films have electron mobilities of up to 21 cm² V^?1 s^?1, a conductivity of 245 S cm^?1, and <5% absorptance in the visible range of the spectrum. The high electron mobilities and low surface roughness (<0.2 nm) are achieved by producing dense and void‐free amorphous layers as confirmed by transmission electron microscopy. These ZTO layers are evaluated for OLEDs in two anode configurations: i) 10 cm² devices with ZTO/Ag/ZTO and ii) 41 cm² devices with ZTO plus a metal grid. The ZTO layers are compatible with OLED processing steps and large‐area white OLEDs fabricated with the ZTO/grid anode show better performance than those with ITO/grid anodes. These results confirm that ZTO has the potential as an In‐free and Earth‐abundant alternative to ITO for large‐area flexible OLEDs.     

Stretchable,Transparent, and Self‐Patterned Hydrogel‐Based Pressure Sensor for Human Motions Detection

In this study, a binary networked conductive hydrogel is prepared using acrylamide and polyvinyl alcohol. Based on the obtained hydrogel, an ultrastretchable pressure sensor with biocompatibility and transparency is fabricated cost effectively. The hydrogel exhibits impressive stretchability (>500%) and superior transparency (>90%). Furthermore, the self‐patterned microarchitecture on the hydrogel surface is beneficial to achieve high sensitivity (0.05 kPa^?1 for 0–3.27 kPa). The hydrogel‐based pressure sensor can precisely monitor dynamic pressures (3.33, 5.02, and 6.67 kPa) with frequency‐dependent behavior. It also shows fast response (150 ms), durable stability (500 dynamic cycles), and negligible current variation (6%). Moreover, the sensor can instantly detect both tiny (phonation, airflowing, and saliva swallowing) and robust (finger and limb motions) physiological activities. This work presents insights into preparing multifunctional hydrogels for mechanosensory electronics.     

Inverted Layer‐By‐Layer Fabrication of an Ultraflexible and Transparent Ag Nanowire/Conductive Polymer Composite Electrode for Use in High‐Performance Organic Solar Cells

A highly flexible and transparent conductive electrode based on consecutively stacked layers of conductive polymer (CP) and silver nanowires (AgNWs) fully embedded in a colorless polyimide (cPI) is achieved by utilizing an inverted layer‐by‐layer processing method. This CP‐AgNW composite electrode exhibits a high transparency of >92% at wavelengths of 450–700 nm and a low resistivity of 7.7 Ω ?^?1, while its ultrasmooth surface provides a large contact area for conductive pathways. Furthermore, it demonstrates an unprecedentedly high flexibility and good mechanical durability during both outward and inward bending to a radius of 40 μm. Subsequent application of this composite electrode in organic solar cells achieves power conversion efficiencies as high as 7.42%, which represents a significant improvement over simply embedding AgNWs in cPI. This is attributed to a reduction in bimolecular recombination and an increased charge collection efficiency, resulting in performance comparable to that of indium tin oxide‐based devices. More importantly, the high mechanical stability means that only a very slight reduction in efficiency is observed with bending (<5%) to a radius of 40 μm. This newly developed composite electrode is therefore expected to be directly applicable to a wide range of high‐performance, low‐cost flexible electronic devices.     

Stretchable and Transparent Biointerface Using Cell‐Sheet–Graphene Hybrid for Electrophysiology and Therapy of Skeletal Muscle

Implantable electronic devices for recording electrophysiological signals and for stimulating muscles and nerves have been widely used throughout clinical medicine. Mechanical mismatch between conventional rigid biomedical devices and soft curvilinear tissues, however, has frequently resulted in a low signal to noise ratio and/or mechanical fatigue and scarring. Multifunctionality ranging from various sensing modalities to therapeutic functions is another important goal for implantable biomedical devices. Here, a stretchable and transparent medical device using a cell‐sheet–graphene hybrid is reported, which can be implanted to form a high quality biotic/abiotic interface. The hybrid is composed of a sheet of C2C12 myoblasts on buckled, mesh‐patterned graphene electrodes. The graphene electrodes monitor and actuate the C2C12 myoblasts in vitro, serving as a smart cell culture substrate that controls their aligned proliferation and differentiation. This stretchable and transparent cell‐sheet–graphene hybrid can be transplanted onto the target muscle tissue, to record electromyographical signals, and stimulate implanted sites electrically and/or optically in vivo. Additional cellular therapeutic effect of the cell‐sheet–graphene hybrid is obtained by integrated myobalst cell sheets. Any immune responses within implanted muscle tissues are not observed. This multifunctional device provides many new opportunities in the emerging field of soft bioelectronics.     

Highly Stretchable or Transparent Conductor Fabrication by a Hierarchical Multiscale Hybrid Nanocomposite

As is frequently seen in sci‐fi movies, future electronics are expected to ultimately be in the form of wearable electronics. To realize wearable electronics, the electric components should be soft, flexible, and even stretchable to be human‐friendly. An important step is presented toward realization of wearable electronics by developing a hierarchical multiscale hybrid nanocomposite for highly flexible, stretchable, or transparent conductors. The hybrid nanocomposite combines the enhanced mechanical compliance, electrical conductivity, and optical transparency of small CNTs (d ≈ 1.2 nm) and the enhanced electrical conductivity of relatively bigger Ag nanowire (d ≈ 150 nm) backbone to provide efficient multiscale electron transport path with Ag nanowire current backbone collector and local CNT percolation network. The highly elastic hybrid nanocomposite conductors and highly transparent flexible conductors can be mounted on any non‐planar or soft surfaces to realize human‐friendly electronics interface for future wearable electronics.     

Role of Polymeric Metal Nucleation Inducers in Fabricating Large‐Area,Flexible, and Transparent Electrodes for Printable Electronics

The advent of special types of transparent electrodes, known as “ultrathin metal electrodes,” opens a new avenue for flexible and printable electronics based on their excellent optical transparency in the visible range while maintaining their intrinsic high electrical conductivity and mechanical flexibility. In this new electrode architecture, introducing metal nucleation inducers (MNIs) on flexible plastic substrates is a key concept to form high‐quality ultrathin metal films (thickness ≈ 10 nm) with smooth and continuous morphology. Herein, this paper explores the role of “polymeric” MNIs in fabricating ultrathin metal films by employing various polymers with different surface energies and functional groups. Moreover, a scalable approach is demonstrated using the ionic self‐assembly on typical plastic substrates, yielding large‐area electrodes (21 × 29.7 cm²) with high optical transmittance (>95%), low sheet resistance (<10 Ω sq^?1), and extreme mechanical flexibility. The results demonstrate that this new class of flexible and transparent electrodes enables the fabrication of efficient polymer light‐emitting diodes.     

Optically Transparent and Mechanically Robust Ionic Hydrogel Electrodes for Bright Electroluminescent Devices Achieving High Stretchability Over 1400%

To realize wearable displays and interactive soft robots, significant research efforts are focused on developing highly deformable alternating-current electroluminescent (ACEL) devices. Although soft emission layers are well developed, designing stretchable, conductive, and transparent soft electrodes remains challenging. In this study, ionic hydrogels are prepared comprising a double network (DN) of poly(N-hydroxyethylacrylamide-co-acrylamide)/crosslinked chitosan swollen in aqueous lithium bis(trifluoromethanesulfonyl) imide. Owing to the finely tuned DN structure of the polymeric crosslinker and transparent electrolyte, the developed ionic hydrogels exhibit remarkable stretchability (1400%), excellent optical transmittance (>99%), and high conductivity (1.95 × 10⁻² Sm⁻¹). Based on the high performance of the ionic hydrogels, ACEL devices are fabricated with an emission layer containing phosphor microparticles and demonstrate stable, high luminance under extreme deformation, and ultra-high elongation. The excellent transparency of the ionic hydrogel further enables the fabrication of novel soft ACEL devices with tandem structures by stacking several emission and electrode layers, in which each emission layer is independently controlled with a switch circuit.     

A Microfluidic,Reversibly Stretchable,Large‐Area Wireless Strain Sensor

This article describes the implementation and characterization of a new self‐contained large‐area wireless strain sensor, operating around 1.5 GHz, based on the concept of multi‐layer microfluidic stretchable radiofrequency electronics (μFSRFEs). Compared to existing solutions, the presented integrated strain sensor is capable of remotely detecting repeated high tensile dynamic strains of up to 15% over very large surfaces or movable parts, and gets rid of all hardwiring to external storage or data processing equipment. Unlike conventional electronic devices, the major part of the sensor is a mechanically reconfigurable and reversibly deformable patch antenna, which consists of two layers of liquid metal alloy filled microfluidic channels in a silicone elastomer. A simplified radiofrequency (RF) transmitter composed of miniaturized rigid active integrated circuits (ICs) associated with discrete passive components was assembled on a flexible printed circuit board (FPCB) and then heterogeneously integrated to the antenna. The elastic patch antenna can withstand repeated mechanical stretches while still maintaining its electrical function to some extent, and return to its original state after removal of the stress. Additionally, its electrical characteristics at frequency of operation are highly sensitive to mechanical strains. Consequently, not only is this antenna a radiator for transmitting and receiving RF signals like any other conventional antennas, but also acts as a reversible large‐area strain sensor in the integrated device. Good electrical performance of the standalone antenna and the RF transmitter sub‐module was respectively verified by experiments. Furthermore, a personal computer (PC)‐assisted RF receiver for receiving and processing the measured data was also designed, implemented, and evaluated. In the real‐life demonstration, the integrated strain sensor successfully monitored periodically repeated human body motion, and wirelessly transmitted the measured data to the custom‐designed receiver at a distance of 5m in real‐time.     

All‐Solution‐Processed Indium‐Free Transparent Composite Electrodes based on Ag Nanowire and Metal Oxide for Thin‐Film Solar Cells

Fully solution‐processed Al‐doped ZnO/silver nanowire (AgNW)/Al‐doped ZnO/ZnO multi‐stacked composite electrodes are introduced as a transparent, conductive window layer for thin‐film solar cells. Unlike conventional sol–gel synthetic pathways, a newly developed combustion reaction‐based sol–gel chemical approach allows dense and uniform composite electrodes at temperatures as low as 200 °C. The resulting composite layer exhibits high transmittance (93.4% at 550 nm) and low sheet resistance (11.3 Ω sq^‐1), which are far superior to those of other solution‐processed transparent electrodes and are comparable to their sputtered counterparts. Conductive atomic force microscopy reveals that the multi‐stacked metal‐oxide layers embedded with the AgNWs enhance the photocarrier collection efficiency by broadening the lateral conduction range. This as‐developed composite electrode is successfully applied in Cu(In_1‐x,Ga_x)S₂ (CIGS) thin‐film solar cells and exhibits a power conversion efficiency of 11.03%. The fully solution‐processed indium‐free composite films demonstrate not only good performance as transparent electrodes but also the potential for applications in various optoelectronic and photovoltaic devices as a cost‐effective and sustainable alternative electrode.     

Stretchable,Transparent, and Thermally Stable Triboelectric Nanogenerators Based on Solvent‐Free Ion‐Conducting Elastomer Electrodes

The development of stretchable/soft electronics requires power sources that can match their stretchability. In this study, a highly stretchable, transparent, and environmentally stable triboelectric nanogenerator with ionic conductor electrodes (iTENG) is reported. The ion‐conducting elastomer (ICE) electrode, together with a dielectric elastomer electrification layer, allows the ICE‐iTENG to achieve a stretchability of 1036% and transmittance of 91.5%. Most importantly, the ICE is liquid solvent‐free and thermally stable up to 335 °C, avoiding the dehydration‐induced performance degradation of commonly used hydrogels. The ICE‐iTENG shows no decrease in electrical output even after storing at 100 °C for 15 h. Biomechanical motion energies are demonstrated to be harvested by the ICE‐iTENG for powering wearable electronics intermittently without extra power sources. An ICE‐iTENG‐based pressure sensor is also developed with sensitivity up to 2.87 kPa^?1. The stretchable ICE‐iTENG overcomes the strain‐induced performance degradation using percolated electrical conductors and liquid evaporation‐induced degradation using ion‐conducting hydrogels/ionogels, suggesting great promising applications in soft/stretchable electronics under a relatively wider temperature range.     

Nature‐Inspired Metallic Networks for Transparent Electrodes

Nature offers structural solutions to various optimization problems. For example, an optimal, low‐shedding water transport at various scales is achieved with quasi‐fractal structures, shown to be close to optimal. In a series of projects, metallic network analogs of some of these solutions to make high‐efficiency transparent conductors are studied. Specifically, transparent conductors are developed by directly metalizing leaf venations, spider webs, and other organic fibers. Also, the natural process of self‐cracking, similar to that occurring in the mud of dried‐out riverbeds, is employed to develop masks for metallic network fabrications. These comprehensive studies and developments contributed to, and in some cases initiate new directions in the field of network transparent conductors. These structures offer performance exceeding those of conventional oxide‐based films, while providing a possibility of reduced processing expense. This paper provides a concise, comparative review of this study and other groups' efforts in recent years. In the context of applications, the performance criteria are defined, and with those as a guideline, practicality of the most promising networks is discussed.     

High‐Performance Hazy Silver Nanowire Transparent Electrodes through Diameter Tailoring for Semitransparent Photovoltaics

Solution‐processed metal nanowire networks have attracted substantial attention as clear transparent conductive electrodes (TCEs) to replace metal oxides for low‐cost and flexible touch panels and displays. While targeting photovoltaic applications, TCEs are expected to be more hazy for enhancing light absorption in the active layer, but are still required to retain high transmittance and low sheet resistance. Balancing these properties (haze, transmittance, and conductivity) in TCEs to realize high performance but high haze simultaneously is a challenge because they are mutually influenced. Here, by precisely tailoring the diameter of thick–long silver nanowires using rapid radial electrochemical etching, high hazy flexible TCEs are fabricated with high figure of merit of up to 741 (4 Ω sq^?1 at 88.4% transmittance with haze of 13.3%), surpassing those of commercialized brittle hazy metal oxides and exhibiting superiority for photovoltaic applications. Laminating such TCEs onto the perovskite solar cells as top electrodes, the obtained semitransparent devices exhibit power efficiencies up to 16.03% and 11.12% when illuminated from the bottom and top sides, respectively, outperforming reported results based on similar device architecture. This study provides a simple strategy for flexible and hazy TCEs fabrication, which is compatible with mild solution‐processed photovoltaic devices, especially those containing heat‐sensitive or chemical‐sensitive materials.