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Skin-like intrinsically stretchable soft electronic devices are essential to realize next-generation remote and preventative medicine for advanced personal healthcare1-4. The recent development of intrinsically stretchable conductors and semiconductors has enabled highly mechanically robust and skin-conformable electronic circuits or optoelectronic devices2,5-10. However, their operating frequencies have been limited to less than 100 hertz, which is much lower than that required for many applications. Here we report intrinsically stretchable diodes-based on stretchable organic and nanomaterials-capable of operating at a frequency as high as 13.56 megahertz. This operating frequency is high enough for the wireless operation of soft sensors and electrochromic display pixels using radiofrequency identification in which the base-carrier frequency is 6.78 megahertz or 13.56 megahertz. This was achieved through a combination of rational material design and device engineering. Specifically, we developed a stretchable anode, cathode, semiconductor and current collector that can satisfy the strict requirements for high-frequency operation. Finally, we show the operational feasibility of our diode by integrating it with a stretchable sensor, electrochromic display pixel and antenna to realize a stretchable wireless tag. This work is an important step towards enabling enhanced functionalities and capabilities for skin-like wearable electronics. Agency for Science, Technology and Research (A*STAR) This work was partially supported by SAIT, Samsung Electronics Co., Ltd., and the Agency for Science, Technology and Research (A*STAR) under its Advanced Manufacturing and Engineering (AME) Programmatic Scheme (no. A18A1b0045). N.M. was partially supported by a Japan Society for the Promotion of Science (JSPS) overseas research fellowship. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. Experiments performed during revision were carried out in Keio University and was supported by JST, PRESTO Grant Number JPMJPR20B7, Japan.

Intrinsically stretchable electronics can form intimate interfaces with the human body, creating devices that could be used to monitor physiological signals without constraining movement. However, mechanical strain invariably leads to the degradation of the electronic properties of the devices. Here we show that strain-insensitive intrinsically stretchable transistor arrays can be created using an all-elastomer strain engineering approach, in which the patterned elastomer layers with tunable stiffnesses are incorporated into the transistor structure. By varying the cross-linking density of the elastomers, areas of increased local stiffness are introduced, reducing strain on the active regions of the devices. This approach can be readily incorporated into existing fabrication processes, and we use it to create arrays with a device density of 340 transistors cm–2 and a strain insensitivity of less than 5% performance variation when stretched to 100% strain. We also show that it can be used to fabricate strain-insensitive circuit elements, including NOR gates, ring oscillators and high-gain amplifiers for the stable monitoring of electrophysiological signals. An all-elastomer strain engineering approach, which uses patterned elastomer layers with tunable stiffnesses, can be used to create intrinsically stretchable transistor arrays with a device density of 340 transistors cm–2 and strain insensitivity of less than 5% performance variation when stretched to 100% strain.

Next-generation wearable electronics require enhanced mechanical robustness and device complexity. Besides previously reported softness and stretchability, desired merits for practical use include elasticity, solvent resistance, facile patternability and high charge carrier mobility. Here, we show a molecular design concept that simultaneously achieves all these targeted properties in both polymeric semiconductors and dielectrics, without compromising electrical performance. This is enabled by covalently-embedded in-situ rubber matrix (iRUM) formation through good mixing of iRUM precursors with polymer electronic materials, and finely-controlled composite film morphology built on azide crosslinking chemistry which leverages different reactivities with C–H and C=C bonds. The high covalent crosslinking density results in both superior elasticity and solvent resistance. When applied in stretchable transistors, the iRUM-semiconductor film retained its mobility after stretching to 100% strain, and exhibited record-high mobility retention of 1 cm2 V−1 s−1 after 1000 stretching-releasing cycles at 50% strain. The cycling life was stably extended to 5000 cycles, five times longer than all reported semiconductors. Furthermore, we fabricated elastic transistors via consecutively photo-patterning of the dielectric and semiconducting layers, demonstrating the potential of solution-processed multilayer device manufacturing. The iRUM represents a molecule-level design approach towards robust skin-inspired electronics., Next-generation skin-inspired electronics require enhanced mechanical robustness and device complexity including elasticity, solvent resistance, and facile patternability. Here, the authors show a molecular design concept that simultaneously achieves all these requirements by covalently linking an in-situ formed rubber matrix with polymer electronic materials.

Biological systems have the powerful ability to self-heal. Human skin can, for example, autonomously heal from wounds of various degrees, allowing it to restore its mechanical and electrical properties. In contrast, human-made electronic devices degrade over time due to fatigue, corrosion or damage incurred during operation, leading to device failure. Self-healing chemistry has emerged in recent years as a promising method for constructing soft electronic materials that are mechanically robust and can self-repair. Here we review the development of self-healing electronic materials and examine how such materials can be used to fabricate self-healing electronic devices. We explore the potential new functionalities of self-healing electronic systems that would not typically be possible with conventional electronic systems and discuss the current challenges in delivering self-healing soft electronics for practical applications. This Review Article examines the development of self-healing electronic materials and devices, explores their potential applications and discusses the challenges that exist in delivering practical systems.

Narrowing the mechanical mismatch between tissue and implantable microelectronics is essential for reducing immune responses and for accommodating body movement. However, the design of implantable soft electronics (on the order of 10 kPa in modulus) remains a challenge because of the limited availability of suitable electronic materials. Here, we report electrically conductive hydrogel-based elastic microelectronics with Young’s modulus values in the kilopascal range. The system consists of a highly conductive soft hydrogel as a conductor and an elastic fluorinated photoresist as the passivation insulation layer. Owing to the high volumetric capacitance and the passivation layer of the hydrogel, electrode arrays of the thin-film hydrogel ‘elastronics’, 20 μm in feature size, show a significantly reduced interfacial impedance with tissue, a current-injection density that is ~30 times higher than that of platinum electrodes, and stable electrical performance under strain. We demonstrate the use of the soft elastronic arrays for localized low-voltage electrical stimulation of the sciatic nerve in live mice. Conductive and elastic hydrogel-based microelectronic arrays with high current-injection density and low interfacial impedance with tissue enable the localized low-voltage electrical stimulation of the sciatic nerve in live mice.

As a key component in stretchable electronics, semiconducting polymers have been widely studied. However, it remains challenging to achieve stretchable semiconducting polymers with high mobility and mechanical reversibility against repeated mechanical stress. Here, we report a simple and universal strategy to realize intrinsically stretchable semiconducting polymers with controlled multi-scale ordering to address this challenge. Specifically, incorporating two types of randomly distributed co-monomer units reduces overall crystallinity and longer-range orders while maintaining short-range ordered aggregates. The resulting polymers maintain high mobility while having much improved stretchability and mechanical reversibility compared with the regular polymer structure with only one type of co-monomer units. Interestingly, the crystalline microstructures are mostly retained even under strain, which may contribute to the improved robustness of our stretchable semiconductors. The proposed molecular design concept is observed to improve the mechanical properties of various p- and n-type conjugated polymers, thus showing the general applicability of our approach. Finally, fully stretchable transistors fabricated with our newly designed stretchable semiconductors exhibit the highest and most stable mobility retention capability under repeated strains of 1,000 cycles. Our general molecular engineering strategy offers a rapid way to develop high mobility stretchable semiconducting polymers., Designing intrinsically stretchable semiconducting polymers with suitable charge transport and mechanical properties required for stretchable electronic devices remains a challenge. Here, the authors report terpolymer-based semiconductors with intrinsically high stretchability and mobility.

Intrinsically and fully stretchable active-matrix-driven displays are an important element to skin electronics that can be applied to many emerging fields, such as wearable electronics, consumer electronics and biomedical devices. Here, we show for the first time a fully stretchable active-matrix-driven organic light-emitting electrochemical cell array. Briefly, it is comprised of a stretchable light-emitting electrochemical cell array driven by a solution-processed, vertically integrated stretchable organic thin-film transistor active-matrix, which is enabled by the development of chemically-orthogonal and intrinsically stretchable dielectric materials. Our resulting active-matrix-driven organic light-emitting electrochemical cell array can be readily bent, twisted and stretched without affecting its device performance. When mounted on skin, the array can tolerate to repeated cycles at 30% strain. This work demonstrates the feasibility of skin-applicable displays and lays the foundation for further materials development., To realize a skin-like display for human-electronics interfaces, intrinsically stretchable light-emitting, transistor and device interconnect components are needed. Here, the authors report a fully stretchable transistor driven active-matrix organic light-emitting electrochemical cell array.

For miniaturized capacitive energy storage, volumetric and areal capacitances are more important metrics than gravimetric ones because of the constraints imposed by device volume and chip area. Typically used in commercial supercapacitors, porous carbons, although they provide a stable and reliable performance, lack volumetric performance because of their inherently low density and moderate capacitances. Here we report a high-performing electrode based on conductive hexaaminobenzene (HAB)-derived two-dimensional metal−organic frameworks (MOFs). In addition to possessing a high packing density and hierarchical porous structure, these MOFs also exhibit excellent chemical stability in both acidic and basic aqueous solutions, which is in sharp contrast to conventional MOFs. Submillimetre-thick pellets of HAB MOFs showed high volumetric capacitances up to 760 F cm−3 and high areal capacitances over 20 F cm−2. Furthermore, the HAB MOF electrodes exhibited highly reversible redox behaviours and good cycling stability with a capacitance retention of 90% after 12,000 cycles. These promising results demonstrate the potential of using redox-active conductive MOFs in energy-storage applications. Metal–organic frameworks (MOFs) are attractive electrodes for supercapacitors but generally suffer from low electric conductivity and chemical stability. Here the authors report stable conductive MOFs based on hexaminobenzene linker with volumetric and areal capacitances in excess of 700 F per cm3 and 15 F per cm2, respectively.

Introducing non-covalent crosslinking moieties to polymer semiconductors produces a stretchable and healable material suitable for wearable electronics. There is great interest and potential in the development of skin-inspired flexible and wearable electronic devices. Such devices require materials that twist, fold and bend with no loss in electronic—or material—properties. Zhenan Bao and colleagues report a conjugated polymer that also incorporates non-covalent interactions between adjacent chains, enabling the material to accommodate up to 100% strain whilst maintaining high charge-carrier mobility. In this proof-of-principle study the authors use the polymers to fabricate flexible and stretchable organic transistors that combine robustness with good electronic properties. Thin-film field-effect transistors are essential elements of stretchable electronic devices for wearable electronics1,2. All of the materials and components of such transistors need to be stretchable and mechanically robust3,4. Although there has been recent progress towards stretchable conductors5,6,7,8, the realization of stretchable semiconductors has focused mainly on strain-accommodating engineering of materials, or blending of nanofibres or nanowires into elastomers9,10,11. An alternative approach relies on using semiconductors that are intrinsically stretchable, so that they can be fabricated using standard processing methods12. Molecular stretchability can be enhanced when conjugated polymers, containing modified side-chains and segmented backbones, are infused with more flexible molecular building blocks13,14. Here we present a design concept for stretchable semiconducting polymers, which involves introducing chemical moieties to promote dynamic non-covalent crosslinking of the conjugated polymers. These non-covalent crosslinking moieties are able to undergo an energy dissipation mechanism through breakage of bonds when strain is applied, while retaining high charge transport abilities. As a result, our polymer is able to recover its high field-effect mobility performance (more than 1 square centimetre per volt per second) even after a hundred cycles at 100 per cent applied strain. Organic thin-film field-effect transistors fabricated from these materials exhibited mobility as high as 1.3 square centimetres per volt per second and a high on/off current ratio exceeding a million. The field-effect mobility remained as high as 1.12 square centimetres per volt per second at 100 per cent strain along the direction perpendicular to the strain. The field-effect mobility of damaged devices can be almost fully recovered after a solvent and thermal healing treatment. Finally, we successfully fabricated a skin-inspired stretchable organic transistor operating under deformations that might be expected in a wearable device.

High-mobility organic field-effect transistors (OFETs) are the basic units for a variety of high-performance electronic applications. Here, we review recent progress in controlling molecular packing and crystal growth in high-mobility, small molecular organic FETs. Strategies to tune molecular packing of organic semiconductors and their impact on charge transport are described. Methods for the controlled growth of single-crystal organic semiconductors required for large-area device construction are reviewed. Furthermore, the advantages, limitations, and potential of these methods are also discussed.

There has been ongoing keen interest to mold electronic devices into desired shapes and be laid on desired configurable surfaces. In specific, the ability to design materials that can bend, twist, compress and stretch repeatedly, while still able to maintain its full capability as conductors or electrodes, has led to numerous efforts to develop flexible and stretchable (bio)devices that are both technologically challenging and environmentally friendly (e.g. biodegradable). In this review, we highlight several recent significant results that have made impacts toward the field of flexible and stretchable electronics, sensors and power sources.

Some animals, such as the chameleon and cephalopod, have the remarkable capability to change their skin colour. This unique characteristic has long inspired scientists to develop materials and devices to mimic such a function. However, it requires the complex integration of stretchability, colour-changing and tactile sensing. Here we show an all-solution processed chameleon-inspired stretchable electronic skin (e-skin), in which the e-skin colour can easily be controlled through varying the applied pressure along with the applied pressure duration. As such, the e-skin's colour change can also be in turn utilized to distinguish the pressure applied. The integration of the stretchable, highly tunable resistive pressure sensor and the fully stretchable organic electrochromic device enables the demonstration of a stretchable electrochromically active e-skin with tactile-sensing control. This system will have wide range applications such as interactive wearable devices, artificial prosthetics and smart robots., Some animals and insects can change the colour of their skin, but mimicking such function in man-made materials is complex. Here, the authors demonstrate an all-solution processed chameleon-inspired stretchable e-skin capable of interactive colour changes and tactile sensing.

Flexible electronics and optoelectronics have potential applications in energy generation, biomedicine, robotics and displays. Two recent demonstrations of highly stretchable polymer LEDs suggest that commercial devices may soon become viable.

Conjugated polymers, such as polyfluorene and poly(phenylene vinylene), have been used to selectively disperse semiconducting single-walled carbon nanotubes (sc-SWNTs), but these polymers have limited applications in transistors and solar cells. Regioregular poly(3-alkylthiophene)s (rr-P3ATs) are the most widely used materials for organic electronics and have been observed to wrap around SWNTs. However, no sorting of sc-SWNTs has been achieved before. Here we report the application of rr-P3ATs to sort sc-SWNTs. Through rational selection of polymers, solvent and temperature, we achieved highly selective dispersion of sc-SWNTs. Our approach enables direct film preparation after a simple centrifugation step. Using the sorted sc-SWNTs, we fabricate high-performance SWNT network transistors with observed charge-carrier mobility as high as 12 cm(2) V(-1) s(-1) and on/off ratio of10(6). Our method offers a facile and a scalable route for separating sc-SWNTs and fabrication of electronic devices.