A New Facile Route to Flexible and Semi‐Transparent Electrodes Based on Water Exfoliated Graphene and their Single‐Electrode Triboelectric Nanogenerator

Wearable technologies are driving current research efforts to self‐powered electronics, for which novel high‐performance materials such as graphene and low‐cost fabrication processes are highly sought.The integration of high‐quality graphene films obtained from scalable water processing approaches in emerging applications for flexible and wearable electronics is demonstrated. A novel method for the assembly of shear exfoliated graphene in water, comprising a direct transfer process assisted by evaporation of isopropyl alcohol is developed. It is shown that graphene films can be easily transferred to any target substrate such as paper, flexible polymeric sheets and fibers, glass, and Si substrates. By combining graphene as the electrode and poly(dimethylsiloxane) as the active layer, a flexible and semi‐transparent triboelectric nanogenerator (TENG) is demonstrated for harvesting energy. The results constitute a new step toward the realization of energy harvesting devices that could be integrated with a wide range of wearable and flexible technologies, and opens new possibilities for the use of TENGs in many applications such as electronic skin and wearable electronics.     

High‐Mobility Helical Tellurium Field‐Effect Transistors Enabled by Transfer‐Free,Low‐Temperature Direct Growth

The transfer‐free direct growth of high‐performance materials and devices can enable transformative new technologies. Here, room‐temperature field‐effect hole mobilities as high as 707 cm² V^?1 s^?1 are reported, achieved using transfer‐free, low‐temperature (≤120 °C) direct growth of helical tellurium (Te) nanostructure devices on SiO₂/Si. The Te nanostructures exhibit significantly higher device performance than other low‐temperature grown semiconductors, and it is demonstrated that through careful control of the growth process, high‐performance Te can be grown on other technologically relevant substrates including flexible plastics like polyethylene terephthalate and graphene in addition to amorphous oxides like SiO₂/Si and HfO₂. The morphology of the Te films can be tailored by the growth temperature, and different carrier scattering mechanisms are identified for films with different morphologies. The transfer‐free direct growth of high‐mobility Te devices can enable major technological breakthroughs, as the low‐temperature growth and fabrication is compatible with the severe thermal budget constraints of emerging applications. For example, vertical integration of novel devices atop a silicon complementary metal oxide semiconductor platform (thermal budget <450 °C) has been theoretically shown to provide a 10× systems level performance improvement, while flexible and wearable electronics (thermal budget <200 °C) can revolutionize defense and medical applications.     

Laser‐Assisted Large‐Scale Fabrication of All‐Solid‐State Asymmetrical Micro‐Supercapacitor Array

The micro‐supercapacitors are of great value for portable, flexible, and integrated electronic equipments. Here, the large‐scale and integrated asymmetrical micro‐supercapacitor (AMSC) array is fabricated in virtue of the laser direct writing and electrodeposition technology. The AMSC shows the ideal flexibility, high areal specific capacitance (21.8 mF cm^?2), and good rate capability. Moreover, its energy density reaches 12.16 µW h cm^?2, outperforming most micro‐supercapacitors reported previously. Meanwhile, large‐scale series‐connected AMSCs are integrated on the flexible substrates (e.g., indium tin oxide‐polyethylene terephthalate film), which can power a veriety of the commercial electronics. The combination of AMSCs array, solar cell, and electronic device proves the feasibility for practical application in the portable, flexible, and integrated electronic equipments.     

Flexible electronics: 12‐GHz Thin‐Film Transistors on Transferrable Silicon Nanomembranes for High‐Performance Flexible Electronics (Small 22/2010)

Multigigahertz flexible electronics are attractive and have broad applications. A gate‐after‐source/drain fabrication process using preselectively doped single‐crystal silicon nanomembranes (SiNM) is an effective approach to realizing high device speed. However, further downscaling this approach has become difficult in lithography alignment. In this full paper, a local alignment scheme in combination with more accurate SiNM transfer measures for minimizing alignment errors is reported. By realizing 1 μm channel alignment for the SiNMs on a soft plastic substrate, thin‐film transistors with a record speed of 12 GHz maximum oscillation frequency are demonstrated. These results indicate the great potential of properly processed SiNMs for high‐performance flexible electronics.     

Gigahertz Electromagnetic Structures via Direct Ink Writing for Radio‐Frequency Oscillator and Transmitter Applications

Radio‐frequency (RF) electronics, which combine passive electromagnetic devices and active transistors to generate and process gigahertz (GHz) signals, provide a critical basis of ever‐pervasive wireless networks. While transistors are best realized by top‐down fabrication, relatively larger electromagnetic passives are within the reach of printing techniques. Here, direct writing of viscoelastic silver‐nanoparticle inks is used to produce a broad array of RF passives operating up to 45 GHz. These include lumped devices such as inductors and capacitors, and wave‐based devices such as transmission lines, their resonant networks, and antennas. Moreover, to demonstrate the utility of these printed RF passive structures in active RF electronic circuits, they are combined with discrete transistors to fabricate GHz self‐sustained oscillators and synchronized oscillator arrays that provide RF references, and wireless transmitters clocked by the oscillators. This work demonstrates the synergy of direct ink writing and RF electronics for wireless applications.     

Multiresponsive Graphene‐Aerogel‐Directed Phase‐Change Smart Fibers

Wearable devices and systems demand multifunctional units with intelligent and integrative functions. Smart fibers with response to external stimuli, such as electrical, thermal, and photonic signals, etc., as well as offering energy storage/conversion are essential units for wearable electronics, but still remain great challenges. Herein, flexible, strong, and self‐cleaning graphene‐aerogel composite fibers, with tunable functions of thermal conversion and storage under multistimuli, are fabricated. The fibers made from porous graphene aerogel/organic phase‐change materials coated with hydrophobic fluorocarbon resin render a wide range of phase transition temperature and enthalpy (0–186 J g^?1). The strong and compliant fibers are twisted into yarn and woven into fabrics, showing a self‐clean superhydrophobic surface and excellent multiple responsive properties to external stimuli (electron/photon/thermal) together with reversible energy storage and conversion. Such aerogel‐directed smart fibers promise for broad applications in the next‐generation of wearable systems.     

Inkjet‐Printed High‐Performance Flexible Micro‐Supercapacitors with Porous Nanofiber‐Like Electrode Structures

Flexible planar micro‐supercapacitors (MSCs) with unique loose and porous nanofiber‐like electrode structures are fabricated by combining electrochemical deposition with inkjet printing. Benefiting from the resulting porous nanofiber‐like structures, the areal capacitance of the inkjet‐printed flexible planar MSCs is obviously enhanced to 46.6 mF cm^?2, which is among the highest values ever reported for MSCs. The complicated fabrication process is successfully averted as compared with previously reported best‐performing planar MSCs. Besides excellent electrochemical performance, the resultant MSCs also show superior mechanical flexibility. The as‐fabricated MSCs can be highly bent to 180° 1000 times with the capacitance retention still up to 86.8%. Intriguingly, because of the remarkable patterning capability of inkjet printing, various modular MSCs in serial and in parallel can be directly and facilely inkjet‐printed without using external metal interconnects and tedious procedures. As a consequence, the electrochemical performance can be largely enhanced to better meet the demands of practical applications. Additionally, flexible serial MSCs with exquisite and aesthetic patterns are also inkjet‐printed, showing great potential in fashionable wearable electronics. The results suggest a feasible strategy for the facile and cost‐effective fabrication of high‐performance flexible MSCs via inkjet printing.     

Flexible Zn‐Ion Batteries: Recent Progresses and Challenges

To keep pace with the increasing pursuit of portable and wearable electronics, it is urgent to develop advanced flexible power supplies. In this context, Zn‐ion batteries (ZIBs) have garnered increasing attention as favorable energy storage devices for flexible electronics, owing to the high capacity, low cost, abundant resources, high safety, and eco‐friendliness. Extensive efforts have been devoted to developing flexible ZIBs in the last few years. This work summarizes the recent achievements in the design, fabrication, and characterization of flexible ZIBs. Representative structures, such as sandwich and cable type, are particularly highlighted. Special emphasis is put on the novel design of electrolyte and electrode, which aims to endow reliable flexibility to the fabricated ZIBs. Moreover, current challenges and future opportunities for the development of high‐performance flexible ZIBs are also outlined.     

Tattoo‐Paper Transfer as a Versatile Platform for All‐Printed Organic Edible Electronics

The use of natural or bioinspired materials to develop edible electronic devices is a potentially disruptive technology that can boost point‐of‐care testing. The technology exploits devices that can be safely ingested, along with pills or even food, and operated from within the gastrointestinal tract. Ingestible electronics can potentially target a significant number of biomedical applications, both as therapeutic and diagnostic tool, and this technology may also impact the food industry, by providing ingestible or food‐compatible electronic tags that can “smart” track goods and monitor their quality along the distribution chain. Temporary tattoo‐paper is hereby proposed as a simple and versatile platform for the integration of electronics onto food and pharmaceutical capsules. In particular, the fabrication of all‐printed organic field‐effect transistors on untreated commercial tattoo‐paper, and their subsequent transfer and operation on edible substrates with a complex nonplanar geometry is demonstrated.     

Advanced Carbon for Flexible and Wearable Electronics

Flexible and wearable electronics are attracting wide attention due to their potential applications in wearable human health monitoring and care systems. Carbon materials have combined superiorities such as good electrical conductivity, intrinsic and structural flexibility, light weight, high chemical and thermal stability, ease of chemical functionalization, as well as potential mass production, enabling them to be promising candidate materials for flexible and wearable electronics. Consequently, great efforts are devoted to the controlled fabrication of carbon materials with rationally designed structures for applications in next‐generation electronics. Herein, the latest advances in the rational design and controlled fabrication of carbon materials toward applications in flexible and wearable electronics are reviewed. Various carbon materials (carbon nanotubes, graphene, natural‐biomaterial‐derived carbon, etc.) with controlled micro/nanostructures and designed macroscopic morphologies for high‐performance flexible electronics are introduced. The fabrication strategies, working mechanism, performance, and applications of carbon‐based flexible devices are reviewed and discussed, including strain/pressure sensors, temperature/humidity sensors, electrochemical sensors, flexible conductive electrodes/wires, and flexible power devices. Furthermore, the integration of multiple devices toward multifunctional wearable systems is briefly reviewed. Finally, the existing challenges and future opportunities in this field are summarized.     

2D Crystal–Based Fibers: Status and Challenges

2D crystals are emerging new materials in multidisciplinary fields including condensed state physics, electronics, energy, environmental engineering, and biomedicine. To employ 2D crystals for practical applications, these nanoscale crystals need to be processed into macroscale materials, such as suspensions, fibers, films, and 3D macrostructures. Among these macromaterials, fibers are flexible, knittable, and easy to use, which can fully reflect the advantages of the structure and properties of 2D crystals. Therefore, the fabrication and application of 2D crystal–based fibers is of great importance for expanding the impact of 2D crystals. In this Review, 2D crystals that are successfully prepared are overviewed based on their composition of elements. Subsequently, methods for preparing 2D crystals, 2D crystals dispersions, and 2D crystal–based fibers are systematically introduced. Then, the applications of 2D crystal–based fibers, such as flexible electronic devices, high‐efficiency catalysis, and adsorption, are also discussed. Finally, the status‐of‐quo, perspectives, and future challenges of 2D crystal–based fibers are summarized. This Review provides directions and guidelines for developing new 2D crystal–based fibers and exploring their potentials in the fields of smart wearable devices.     

Roll‐to‐Roll Production of Graphene Hybrid Electrodes for High‐Efficiency,Flexible Organic Photoelectronics

Despite nearly two decades of research, the absence of ideal, flexible, and transparent electrodes has been the biggest bottleneck for realizing flexible and printable electronics via roll‐to‐roll (R2R) method. A fabrication of poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate):graphene:ethyl cellulose (PEDOT:PSS:G:EC) hybrid electrodes by R2R process, which allows for the elimination of strong acid treatment. The high‐performance flexible printable electrode includes a transmittance (T) of 78% at 550 nm and a sheet resistance of 13 Ω sq⁻¹ with excellent mechanical stability. These features arise from the PSS interacting strongly with the ethyoxyl groups from EC promoting a favorable phase separation between PEDOT and PSS chains, and the highly uniform and conductive G:EC enable rearrangement of the PEDOT chains with more expanded conformation surrounded by G:EC via the π–π interaction between G:EC and PEDOT. The hybrid electrodes are fully functional as universal electrodes for outstanding flexible electronic applications. Organic solar cells based on the hybrid electrode exhibit a high power conversion efficiency of 9.4% with good universality for active layer. Moreover, the organic light‐emitting diodes and photodetector devices hold the same level to or outperform those based on indium tin oxide flexible transparent electrodes.     

Grain‐Boundary‐Induced Drastic Sensing Performance Enhancement of Polycrystalline‐Microwire Printed Gas Sensors

The development of materials with high efficiency and stable signal output in a bent state is important for flexible electronics. Grain boundaries provide lasting inspiration and a promising avenue for designing advanced functionalities using nanomaterials. Combining bulk defects in polycrystalline materials is shown to result in rich new electronic structures, catalytic activities, and mechanical properties for many applications. However, direct evidence that grain boundaries can create new physicochemical properties in flexible electronics is lacking. Here, a combination of bulk electrosensitive measurements, density functional theory calculations, and atomic force microscopy technology with quantitative nanomechanical mapping is used to show that grain boundaries in polycrystalline wires are more active and mechanically stable than single‐crystalline wires for real‐time detection of chemical analytes. The existence of a grain boundary improves the electronic and mechanical properties, which activate and stabilize materials, and allow new opportunities to design highly sensitive, flexible chemical sensors.     

Textile Display for Electronic and Brain‐Interfaced Communications

Textile displays are poised to revolutionize current electronic devices, and reshape the future of electronics and related fields such as biomedicine and soft robotics. However, they remain unavailable due to the difficulty of directly constructing electroluminescent devices onto the textile‐like substrate to really display desired programmable patterns. Here, a novel textile display is developed from continuous electroluminescent fibers made by a one‐step extrusion process. The resulting displaying textile is flexible, stretchable, three‐dimensionally twistable, conformable to arbitrarily curved skins, and breathable, and can dynamically display a series of desired patterns, making it useful for bioinspired electronics, soft robotics, and electroluminescent skins, among other applications. It is demonstrated that these displaying textiles can also communicate with a computer and mouse brain for smart display and camouflage applications. This work may open up a new direction for the integration of wearable electroluminescent devices with the human body, providing new and promising communication platforms.     

Exploring Two‐Dimensional Transport Phenomena in Metal Oxide Heterointerfaces for Next‐Generation,High‐Performance,Thin‐Film Transistor Technologies

In the last decade, metal oxides have emerged as a fascinating class of electronic material, exhibiting a wide range of unique and technologically relevant characteristics. For example, thin‐film transistors formed from amorphous or polycrystalline metal oxide semiconductors offer the promise of low‐cost, large‐area, and flexible electronics, exhibiting performances comparable to or in excess of incumbent silicon‐based technologies. Atomically flat interfaces between otherwise insulating or semiconducting complex oxides, are also found to be highly conducting, displaying 2‐dimensional (2D) charge transport properties, strong correlations, and even superconductivity. Field‐effect devices employing such carefully engineered interfaces are hoped to one day compete with traditional group IV or III–V semiconductors for use in the next‐generation of high‐performance electronics. In this Concept article we provide an overview of the different metal oxide transistor technologies and potential future research directions. In particular, we look at the recent reports of multilayer oxide thin‐film transistors and the possibility of 2D electron transport in these disordered/polycrystalline systems and discuss the potential of the technology for applications in large‐area electronics.     

Monolithic and Flexible ZnS/SnO2 Ultraviolet Photodetectors with Lateral Graphene Electrodes

A continuing trend of miniaturized and flexible electronics/optoelectronic calls for novel device architectures made by compatible fabrication techniques. However, traditional layer‐to‐layer structures cannot satisfy such a need. Herein, a novel monolithic optoelectronic device fabricated by a mask‐free laser direct writing method is demonstrated in which in situ laser induced graphene‐like materials are employed as lateral electrodes for flexible ZnS/SnO₂ ultraviolet photodetectors. Specifically, a ZnS/SnO₂ thin film comprised of heterogeneous ZnS/SnO₂ nanoparticles is first coated on polyimide (PI) sheets by a solution process. Then, CO₂ laser irradiation ablates designed areas of the ZnS/SnO₂ thin film and converts the underneath PI into highly conductive graphene as the lateral electrodes for the monolithic photodetectors. This in situ growth method provides good interfaces between the graphene electrodes and the semiconducting ZnS/SnO₂ resulting in high optoelectronic performance. The lateral electrode structure reduces total thickness of the devices, thus minimizing the strain and improving flexibility of the photodetectors. The demonstrated lithography‐free monolithic fabrication is a simple and cost‐effective method, showing a great potential for developement into roll‐to‐roll manufacturing of flexible electronics.     

3D Direct Laser Writing of Nano‐ and Microstructured Hierarchical Gecko‐Mimicking Surfaces

Applying 3D direct laser writing, artificial hierarchical gecko‐type structures are designed and fabricated down to nanometer dimensions. In this way, the elastic modulus and the length scale of the gecko's setae are very closely matched. Direct laser writing is a very flexible rapid prototyping method allowing the fabrication of arbitrary nanostructures. Since the parameters of the structures can be easily changed, this technique is perfect for design studies of dry adhesives. Measuring the adhesional forces by atomic force microscopy, the influence of several design parameters like density, aspect ratio, and tip‐shape on dry adhesion performance are systematically examined. In this way, it is revealed that hierarchy is favorable for artificial gecko‐inspired dry adhesives made of stiff materials on the nanometer scale.     

From One‐ to Three‐Dimensional Organic Semiconductors: In Search of the Organic Silicon?

Organic semiconductors based on π‐conjugated systems are the focus of considerable interest in the emerging area of soft or flexible photonics and electronics. Whereas in recent years the performances of devices such as organic light‐emitting diodes (OLEDs), organic field‐effect transistors (OFETs), or solar cells have undergone considerable progress, a number of technical and fundamental problems related to the low dimensionality of organic semiconductors based on linear π‐conjugated systems remain unsatisfactorily resolved. This low dimensionality results in an anisotropy of the optical and charge‐transport properties, which in turn implies a control of the material organization/molecular orientation during or after device fabrication. Such a constraint evidently represents a problem when device fabrication by solution‐based processes, such as printing techniques, is envisioned. The aim of this short Review is to illustrate possible alternative strategies based on the development of organic semiconductors with higher dimensionality, capable to exhibit isotropic electronic properties.     

Thread‐like Supercapacitors Based on One‐Step Spun Nanocomposite Yarns

Thread‐like electronic devices have attracted great interest because of their potential applications in wearable electronics. To produce high‐performance, thread‐like supercapacitors, a mixture of stable dispersions of single‐walled carbon nanotubes and conducting polyaniline nanowires are prepared. Then, the mixture is spun into flexible yarns with a polyvinyl alcohol outer sheath by a one‐step spinning process. The composite yarns show excellent mechanical properties and high electrical conductivities after sufficient washing to remove surfactants. After applying a further coating layer of gel electrolyte, two flexible yarns are twisted together to form a thread‐like supercapacitor. The supercapacitor based on these two yarns (SWCNTs and PAniNWs) possesses a much higher specific capacitance than that based only on pure SWCNTs yarns, making it an ideal energy‐storage device for wearable electronics.     

Highly Crystalline C8‐BTBT Thin‐Film Transistors by Lateral Homo‐Epitaxial Growth on Printed Templates

Highly crystalline thin films of organic semiconductors offer great potential for fundamental material studies as well as for realizing high‐performance, low‐cost flexible electronics. The fabrication of these films directly on inert substrates is typically done by meniscus‐guided coating techniques. The resulting layers show morphological defects that hinder charge transport and induce large device‐to‐device variability. Here, a double‐step method for organic semiconductor layers combining a solution‐processed templating layer and a lateral homo‐epitaxial growth by a thermal evaporation step is reported. The epitaxial regrowth repairs most of the morphological defects inherent to meniscus‐guided coatings. The resulting film is highly crystalline and features a mobility increased by a factor of three and a relative spread in device characteristics improved by almost half an order of magnitude. This method is easily adaptable to other coating techniques and offers a route toward the fabrication of high‐performance, large‐area electronics based on highly crystalline thin films of organic semiconductors.