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.     

Local Crack‐Programmed Gold Nanowire Electronic Skin Tattoos for In‐Plane Multisensor Integration

Sensitive, specific, yet multifunctional tattoo‐like electronics are ideal wearable systems for “any time, any where” health monitoring because they can virtually become parts of the human skin, offering a burdenless “unfeelable” wearing experience. A skin‐like, multifunctional electronic tattoo made entirely from gold using a standing enokitake‐mushroom‐like vertically aligned nanowire membrane in conjunction with a programmable local cracking technology is reported. Unlike previous multifunctional systems, only a single material type is needed for the integrated gold circuits involved in interconnects and multiplexed specific sensors, thereby avoiding the use of complex multimaterials interfaces. This is possiblebecause the programmable local cracking technology allows for the arbitrary fine‐tuning of the properties of elastic gold conductors from strain‐insensitive to highly strain‐sensitive simply by adjusting localized crack size, shape, and orientations—a capability impossible to achieve with previous bulk cracking technology. Furthermore, in‐plane integration of strain/pressure sensors, anisotropic orientation‐specific sensors, strain‐insensitive stretchable interconnects, temperature sensors, glucose sensors, and lactate sensors without the need of soldering or gluing are demonstrated. This strategy opens a new general route for the design of next‐generation wearable electronic tattoos.     

Surface‐Embedded Stretchable Electrodes by Direct Printing and their Uses to Fabricate Ultrathin Vibration Sensors and Circuits for 3D Structures

Printing is one of the easy and quick ways to make a stretchable wearable electronics. Conventional printing methods deposit conductive materials “on” or “inside” a rubber substrate. The conductors made by such printing methods cannot be used as device electrodes because of the large surface topology, poor stretchability, or weak adhesion between the substrate and the conducting material. Here, a method is presented by which conductive materials are printed in the way of being surface‐embedded in the rubber substrate; hence, the conductors can be widely used as device electrodes and circuits. The printing process involves a direct printing of a metal precursor solution in a block‐copolymer rubber substrate and chemical reduction of the precursor into metal nanoparticles. The electrical conductivity and sensitivity to the mechanical deformation can be controlled by adjusting the number of printing operations. The fabrication of highly sensitive vibration sensors is thus presented, which can detect weak pulses and sound waves. In addition, this work takes advantage of the viscoelasticity of the composite conductor to fabricate highly conductive stretchable circuits for complicated 3D structures. The printed electrodes are also used to fabricate a stretchable electrochemiluminescence display.     

Ultrastretchable Conductor Fabricated on Skin‐Like Hydrogel–Elastomer Hybrid Substrates for Skin Electronics

Printing technology can be used for manufacturing stretchable electrodes, which represent essential parts of wearable devices requiring relatively high degrees of stretchability and conductivity. In this work, a strategy for fabricating printable and highly stretchable conductors are proposed by transferring printed Ag ink onto stretchable substrates comprising Ecoflex elastomer and tough hydrogel layers using a water‐soluble tape. The elastic modulus of the produced hybrid film is close to that of the hydrogel layer, since the thickness of Ecoflex elastomer film coated on hydrogel is very thin (30 µm). Moreover, the fabricated conductor on hybrid film is stretched up to 1780% strain. The described transfer method is simpler than other techniques utilizing elastomer stamps or sacrificial layers and enables application of printable electronics to the substrates with low elastic moduli (such as hydrogels). The integration of printed electronics with skin‐like low‐modulus substrates can be applied to make wearable devices more comfortable for human skin.     

Breathable Nanowood Biofilms as Guiding Layer for Green On‐Skin Electronics

Thin‐film electronics are urged to be directly laminated onto human skin for reliable, sensitive biosensing together with feedback transdermal therapy, their self‐power supply using the thermoelectric and moisture‐induced‐electric effects also has gained great attention (skin and on‐skin electronics (On‐skinE) themselves are energy storehouses). However, “thin‐film” On‐skinE 1) cannot install “bulky” heatsinks or sweat transport channels, but the output power of thermoelectric generator and moisture‐induced‐electric generator relies on the temperature difference (?T ) across generator and the ambient humidity (AH), respectively; 2) lack a routing and accumulation of sweat for biosensing, lack targeted delivery of drugs for precise transdermal therapy; and 3) need insulation between the heat‐generating unit and heat‐sensitive unit. Here, two breathable nanowood biofilms are demonstrated, which can help insulate between units and guide the heat and sweat to another in‐plane direction. The transparent biofilms achieve record‐high transport_///transport_⊥ (//: along cellulose nanofiber alignment direction, ⊥: perpendicular direction) of heat (925%) and sweat (338%), winning applications emphasizing on ?T/AH‐dependent output power and “reliable” biosensing. The porous biofilms are competent in applications where “sensitive” biosensing (transporting_// sweat up to 11.25 mm s^?1 at the 1st second), “insulating” between units, and “targeted” delivery of saline‐soluble drugs are of uppermost priority.     

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.     

Biodegradable Electronic Systems in 3D,Heterogeneously Integrated Formats

Biodegradable electronic systems represent an emerging class of technology with unique application possibilities, from temporary biomedical implants to “green” consumer gadgets. This paper introduces materials and processing methods for 3D, heterogeneously integrated devices of this type, with various functional examples in sophisticated forms of silicon‐based electronics. Specifically, techniques for performing multilayer assembly by transfer printing and for fabricating layer‐to‐layer vias and interconnects by lithographic procedures serve as routes to biodegradable, 3D integrated circuits composed of functional building blocks formed using specialized approaches or sourced from commercial semiconductor foundries. Demonstration examples range from logic gates and analog circuits that undergo functional transformation by transience to systems that integrate multilayer resistive sensors for in situ, continuous electrical monitoring of the processes of transience. The results significantly expand the scope of engineering options for biodegradable electronics and other types of transient microsystem technologies.     

Stretchable,Large‐area Organic Electronics

Stretchability will significantly expand the application scope of electronics, particularly large‐area electronics—displays, sensors, and actuators. If arbitrary surfaces and movable parts could be covered with stretchable electronics, which is impossible with conventional electronics, new classes of applications are expected to emerge. A large hurdle is manufacturing electrical wiring with high conductivity, high stretchability, and large‐area compatibility. This Review describes stretchable, large‐area electronics based on organic field‐effect transistors for applications to sensors and displays. First, novel net‐shaped organic transistors are employed to realize stretchable, large‐area sensor networks that detect distributions of pressure and temperature simultaneously. The whole system is functional even when it is stretched by 25%. In order to further improve stretchability, printable elastic conductors are developed by dispersing single‐walled carbon nanotubes (SWNTs) as dopants uniformly in rubbers. Further, we describe integration of printable elastic conductors with organic transistors to construct a rubber‐like stretchable active matrix for large‐area sensor and display applications. Finally, we will discuss the future prospects of stretchable, large‐area electronics with delineating a picture of the next‐generation human/machine interfaces from the aspect of materials science and electronic engineering.     

Inkjet‐Printed Lithium–Sulfur Microcathodes for All‐Printed,Integrated Nanomanufacturing

Improved thin‐film microbatteries are needed to provide appropriate energy‐storage options to power the multitude of devices that will bring the proposed “Internet of Things” network to fruition (e.g., active radio‐frequency identification tags and microcontrollers for wearable and implantable devices). Although impressive efforts have been made to improve the energy density of 3D microbatteries, they have all used low energy‐density lithium‐ion chemistries, which present a fundamental barrier to miniaturization. In addition, they require complicated microfabrication processes that hinder cost‐competitiveness. Here, inkjet‐printed lithium–sulfur (Li–S) cathodes for integrated nanomanufacturing are reported. Single‐wall carbon nanotubes infused with electronically conductive straight‐chain sulfur (S@SWNT) are adopted as an integrated current‐collector/active‐material composite, and inkjet printing as a top‐down approach to achieve thin‐film shape control over printed electrode dimensions is used. The novel Li–S cathodes may be directly printed on traditional microelectronic semicoductor substrates (e.g., SiO₂) or on flexible aluminum foil. Profilometry indicates that these microelectrodes are less than 10 µm thick, while cyclic voltammetry analyses show that the S@SWNT possesses pseudocapacitive characteristics and corroborates a previous study suggesting the S@SWNT discharge via a purely solid‐state mechanism. The printed electrodes produce ≈800 mAh g^?1 S initially and ≈700 mAh g^?1 after 100 charge/discharge cycles at C/2 rate.     

Browsing the Real World using Organic Electronics,Si‐Chips,and a Human Touch

Organic electronics have been developed according to an orthodox doctrine advocating “all‐printed’’, “all‐organic’’ and “ultra‐low‐cost’’ primarily targeting various e‐paper applications. In order to harvest from the great opportunities afforded with organic electronics potentially operating as communication and sensor outposts within existing and future complex communication infrastructures, high‐quality computing and communication protocols must be integrated with the organic electronics. Here, we debate and scrutinize the twinning of the signal‐processing capability of traditional integrated silicon chips with organic electronics and sensors, and to use our body as a natural local network with our bare hand as the browser of the physical world. The resulting platform provides a body network, i.e., a personalized web, composed of e‐label sensors, bioelectronics, and mobile devices that together make it possible to monitor and record both our ambience and health‐status parameters, supported by the ubiquitous mobile network and the resources of the “cloud”.     

Covalent Bonding of Thermoplastics to Rubbers for Printable,Reel‐to‐Reel Processing in Soft Robotics and Microfluidics

The lamination of mechanically stiff structures to elastic materials is prevalent in biological systems and popular in many emerging synthetic systems, such as soft robotics, microfluidics, stretchable electronics, and pop‐up assemblies. The disparate mechanical and chemical properties of these materials have made it challenging to develop universal synthetic procedures capable of reliably adhering to these classes of materials together. Herein, a simple and scalable procedure is described that is capable of covalently laminating a variety of commodity (“off‐the‐shelf”) thermoplastic sheets to silicone rubber films. When combined with laser printing, the nonbonding sites can be “printed” onto the thermoplastic sheets, enabling the direct fabrication of microfluidic systems for actuation and liquid handling applications. The versatility of this approach in generating thin, multifunctional laminates is demonstrated through the fabrication of milliscale soft actuators and grippers with hinged articulation and microfluidic channels with built‐in optical filtering and pressure‐dependent geometries. This method of fabrication offers several advantages, including technical simplicity, process scalability, design versatility, and material diversity. The concepts and strategies presented herein are broadly applicable to the soft robotics, microfluidics, and advanced and additive manufacturing communities where hybrid rubber/plastic structures are prevalent.     

Directed Assembly of Liquid Metal–Elastomer Conductors for Stretchable and Self-Healing Electronics

Growing interest in soft robotics, stretchable electronics, and electronic skins has created demand for soft, compliant, and stretchable electrodes and interconnects. Here, dielectrophoresis (DEP) is used to assemble, align, and sinter eutectic gallium indium (EGaIn) microdroplets in uncured poly(dimethylsiloxane) (PDMS) to form electrically conducting microwires. There are several noteworthy aspects of this approach. 1) Generally, EGaIn droplets in silicone at loadings approaching 90 wt% remain insulating and form a conductive network only when subjected to sintering. Here, DEP facilitates assembly of EGaIn droplets into conductive microwires at loadings as low as 10 wt%. 2) DEP is done in silicone for the first time, enabling the microwires to be cured in a stretchable matrix. 3) Liquid EGaIn droplets sinter during DEP to form a stretchable metallic microwire that retains its shape after curing the silicone. 4) Use of liquid metal eliminates the issue of compliance mismatch observed in soft polymers with solid fillers. 5) The silicone–EGaIn “ink” can be assembled by DEP within the crevices of severely damaged wires to create stretchable interconnects that heal the damage mechanically and electrically. The DEP process of this unique set of materials is characterized and the interesting attributes enabled by such liquid microwires are demonstrated.     

Progress Report on “From Printed Electrolyte‐Gated Metal‐Oxide Devices to Circuits”

Printed electrolyte‐gated oxide electronics is an emerging electronic technology in the low voltage regime (≤1 V). Whereas in the past mainly dielectrics have been used for gating the transistors, many recent approaches employ the advantages of solution processable, solid polymer electrolytes, or ion gels that provide high gate capacitances produced by a Helmholtz double layer, allowing for low‐voltage operation. Herein, with special focus on work performed at KIT recent advances in building electronic circuits based on indium oxide, n‐type electrolyte‐gated field‐effect transistors (EGFETs) are reviewed. When integrated into ring oscillator circuits a digital performance ranging from 250 Hz at 1 V up to 1 kHz is achieved. Sequential circuits such as memory cells are also demonstrated. More complex circuits are feasible but remain challenging also because of the high variability of the printed devices. However, the device inherent variability can be even exploited in security circuits such as physically unclonable functions (PUFs), which output a reliable and unique, device specific, digital response signal. As an overall advantage of the technology all the presented circuits can operate at very low supply voltages (0.6 V), which is crucial for low‐power printed electronics applications.     

Human‐Finger Electronics Based on Opposing Humidity‐Resistance Responses in Carbon Nanofilms

Carbon nanomaterials have excellent humidity sensing properties. Here, it is demonstrated that multiwalled carbon‐nanotube (MWCNT)‐ and reduced‐graphene‐oxide (rGO)‐based conductive films have opposite humidity/electrical resistance responses: MWCNTs increase their electrical resistance (positive response) and rGOs decrease their electrical resistance (negative response). The authors propose a new phenomenology that describes a “net”‐like model for MWCNT films and a “scale”‐like model for rGO films to explain these behaviors based on contributions from junction resistances (at interparticle junctions) and intrinsic resistances (of the particles). This phenomenology is accordingly validated via a series of experiments, which complement more classical models based on proton conductivity. To explore the practical applications of the converse humidity/resistance responses, a humidity‐insensitive MWCNT/rGO hybrid conductive films is developed, which has the potential to greatly improve the stability of carbon‐based electrical device to humidity. The authors further investigate the application of such films to human‐finger electronics by fabricating transparent flexible devices consisting of a polyethylene terephthalate substrate equipped with an MWCNT/rGO pattern for gesture recognition, and MWCNT/rGO/MWCNT or rGO/MWCNT/rGO patterns for 3D noncontact sensing, which will be complementary to existing 3D touch technology.     

Ink‐Jet Printed CMOS Electronics from Oxide Semiconductors

Complementary metal oxide semiconductor (CMOS) technology with high transconductance and signal gain is mandatory for practicable digital/analog logic electronics. However, high performance all‐oxide CMOS logics are scarcely reported in the literature; specifically, not at all for solution‐processed/printed transistors. As a major step toward solution‐processed all‐oxide electronics, here it is shown that using a highly efficient electrolyte‐gating approach one can obtain printed and low‐voltage operated oxide CMOS logics with high signal gain (≈21 at a supply voltage of only 1.5 V) and low static power dissipation.     

Stretchable and Tunable Microtectonic ZnO‐Based Sensors and Photonics

The concept of realizing electronic applications on elastically stretchable “skins” that conform to irregularly shaped surfaces is revolutionizing fundamental research into mechanics and materials that can enable high performance stretchable devices. The ability to operate electronic devices under various mechanically stressed states can provide a set of unique functionalities that are beyond the capabilities of conventional rigid electronics. Here, a distinctive microtectonic effect enabled oxygen‐deficient, nanopatterned zinc oxide (ZnO) thin films on an elastomeric substrate are introduced to realize large area, stretchable, transparent, and ultraportable sensors. The unique surface structures are exploited to create stretchable gas and ultraviolet light sensors, where the functional oxide itself is stretchable, both of which outperform their rigid counterparts under room temperature conditions. Nanoscale ZnO features are embedded in an elastomeric matrix function as tunable diffraction gratings, capable of sensing displacements with nanometre accuracy. These devices and the microtectonic oxide thin film approach show promise in enabling functional, transparent, and wearable electronics.     

Silver‐Quantum‐Dot‐Modified MoO3 and MnO2 Paper‐Like Freestanding Films for Flexible Solid‐State Asymmetric Supercapacitors

Free‐standing paper‐like thin‐film electrodes have great potential to boost next‐generation power sources with highly flexible, ultrathin, and lightweight requirements. In this work, silver‐quantum‐dot‐ (2–5 nm) modified transition metal oxide (including MoO₃ and MnO₂) paper‐like electrodes are developed for energy storage applications. Benefitting from the ohmic contact at the interfaces between silver quantum dots and MoO₃ nanobelts (or MnO₂ nanowires) and the binder‐free nature and 0D/1D/2D nanostructured 3D network of the fabricated electrodes, substantial improvements on the electrical conductivity, efficient ionic diffusion, and areal capacitances of the hybrid nanostructure electrodes are observed. With this proposed strategy, the constructed asymmetric supercapacitors, with Ag quantum dots/MoO₃ “paper” as anode, Ag quantum dots/MnO₂ “paper” as cathode, and neutral Na₂SO₄/polyvinyl alcohol hydrogel as electrolyte, exhibit significantly enhanced energy and power densities in comparison with those of the supercapacitors without modification of Ag quantum dots on electrodes; present excellent cycling stability at different current densities and good flexibility under various bending states; offer possibilities as high‐performance power sources with low cost, high safety, and environmental friendly properties.     

Skin‐Like Stretchable Fuel Cell Based on Gold‐Nanowire‐Impregnated Porous Polymer Scaffolds

Skin‐like energy devices can be conformally attached to the human body, which are highly desirable to power soft wearable electronics in the future. Here, a skin‐like stretchable fuel cell based on ultrathin gold nanowires (AuNWs) and polymerized high internal phase emulsions (polyHIPEs) scaffolds is demonstrated. The polyHIPEs can offer a high porosity of 80% yet with an overall thickness comparable to human skin. Upon impregnation with electronic inks containing ultrathin (2 nm in diameter) and ultrahigh aspect‐ratio (>10 000) gold nanowires, skin‐like strain‐insensitive stretchable electrodes are successfully fabricated. With such designed strain‐insensitive electrodes, a stretchable fuel cell is fabricated by using AuNWs@polyHIPEs, platinum (Pt)‐modified AuNWs@polyHIPEs, and ethanol as the anode, cathode, and fuel, respectively. The resulting epidermal fuel cell can be patterned and transferred onto skin as “tattoos” yet can offer a high power density of 280 µW cm^?2 and a high durability (>90% performance retention under stretching, compression, and twisting). The results presented here demonstrate that this skin‐thin, porous, yet stretchable electrode is essentially multifunctional, simultaneously serving as a current collector, an electrocatalyst, and a fuel host, indicating potential applications to power future soft wearable 2.0 electronics for remote healthcare and soft robotics.     

Smart Eutectic Gallium–Indium: From Properties to Applications

Eutectic gallium–indium (EGaIn), a liquid metal with a melting point close to or below room temperature, has attracted extensive attention in recent years due to its excellent properties such as fluidity, high conductivity, thermal conductivity, stretchability, self-healing capability, biocompatibility, and recyclability. These features of EGaIn can be adjusted by changing the experimental condition, and various composite materials with extended properties can be further obtained by mixing EGaIn with other materials. In this review, not only the are unique properties of EGaIn introduced, but also the working principles for the EGaIn-based devices are illustrated and the developments of EGaIn-related techniques are summarized. The applications of EGaIn in various fields, such as flexible electronics (sensors, antennas, electronic circuits), molecular electronics (molecular memory, opto-electronic switches, or reconfigurable junctions), energy catalysis (heat management, motors, generators, batteries), biomedical science (drug delivery, tumor therapy, bioimaging and neural interfaces) are reviewed. Finally, a critical discussion of the main challenges for the development of EGaIn-based techniques are discussed, and the potential applications in new fields are prospected.     

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.