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Printed electronics received a great attention in both research and commercialization since it allows fabrication of low-cost, large area electronic devices on various substrates. Printed electronics plays a critical role in facilitating stretchable electronics since it allows patterning newly developed stretchable conductors which is difficult to be achieved with conventional silicon-based microfabrication technologies, such as photolithography and vacuum-based techniques. To realize printed electronics which is necessary for the development of stretchable electronics, printing technologies, formulation of conductive inks, and integration of functional devices have been widely investigated in the recent years. This review summarizes principles and recent development of printing techniques, materials for stretchable conductors and their applications in stretchable electronics using various printing techniques. The challenge is that only a few researches satisfying both excellent materials properties and good printability were reported. Future efforts will greatly expand the possibilities of using printed electronics for stretchable electronics.

Pressure-sensitive adhesives (PSAs) have been a workhorse in diverse applications from the repair of objects to heavy-duty industrial use due to their unique capability to form near-instant and robust yet repeatable adhesion to a wide range of engineering solids via physical bonding. While these characteristics of PSAs are highly favorable in various biomedical applications, commercial PSAs lack adhesion to wet tissue surfaces. Moreover, existing bioadhesives are mostly limited to single-use applications incapable of repeated adhesion and repositioning due to the irreversible nature of chemical adhesion. In this work, we introduce a pressure-sensitive bioadhesive (PSB) that synergistically combines the advantages of viscoelastic PSAs and bioadhesives. Enabled by a one-pot scalable copolymerization of a poly(glycerol sebacate)-co-poly(ethylene glycol) (PGS-co-PEG) block copolymer, the PSB provides near-instant (~ 1 s), robust, and repeatable (over 1,000 times) adhesion to wet biological tissues (i.e., skin, lung, heart) and engineering (i.e., metals, plastics) substrates without prior surface functionalization. We further demonstrate in vitro and in vivo biocompatibility and biodegradability of the PSB and its potential applications as a surgical sealant and the rapid, robust, and repositionable integration of biomedical devices with wet dynamic organs in rat and porcine models.

The all-hydrogel gripper was composed of three temperature-responsive hydrogels that mimicked the human bone, cartilage, and flexor tendon. With tough adhesion via split-brushing adhesion, our all-hydrogel gripper showed a high load capacity.

Humans rely increasingly on sensors to address grand challenges and to improve quality of life in the era of digitalization and big data. For ubiquitous sensing, flexible sensors are developed to overcome the limitations of conventional rigid counterparts. Despite rapid advancement in bench-side research over the last decade, the market adoption of flexible sensors remains limited. To ease and to expedite their deployment, here, we identify bottlenecks hindering the maturation of flexible sensors and propose promising solutions. We first analyze challenges in achieving satisfactory sensing performance for real-world applications and then summarize issues in compatible sensor-biology interfaces, followed by brief discussions on powering and connecting sensor networks. Issues en route to commercialization and for sustainable growth of the sector are also analyzed, highlighting environmental concerns and emphasizing nontechnical issues such as business, regulatory, and ethical considerations. Additionally, we look at future intelligent flexible sensors. In proposing a comprehensive roadmap, we hope to steer research efforts towards common goals and to guide coordinated development strategies from disparate communities. Through such collaborative efforts, scientific breakthroughs can be made sooner and capitalized for the betterment of humanity. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) Submitted/Accepted version Y.L., Z.L., M.Z., and X.C. acknowledge the National Research Foundation, Singapore (NRF) under NRF’s Medium Sized Centre: Singapore Hybrid-Integrated Next-Generation μElectronics (SHINE) Centre funding programme, and AME programming funding scheme of Cyber Physiochemical Interface (CPI) project (no. A18A1b0045). Y.L. acknowledges National Natural Science Foundation of China (62201243). C.J. acknowledges funding support from the National Key R&D Program of China (no. 2019YFA0706100), the National Natural Science Foundation of China (82151305), Lingang Laboratory (LG-QS-202202-09). T.Q.T. and N.E.L. acknowledge support by the Basic Science Research Program (no. 2020R1A2C3013480) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT. A.F. acknowledges the AFOSR (grant FA9550-22-1-0423). Y.L. and Y.Z. would like to acknowledge the NSF (award no. 2134664) and NIH (award no. R01HD108473) for financial support. X.F. acknowledges the support from the National Natural Science Foundation of China (grant no. U20A6001). L.Y. would like to thank the A*STAR Central Research Fund (CRF) and the AME Programmatic A18A1b0045 (Cyber Physiochemical Interfaces) for funding support. C.F.G. acknowledges the National Natural Science Foundation of China (no. T2225017). T.Q.T. acknowledges the Brain Pool Program (No. 2020H1D3A2A02111068) through the National Research Foundation (NRF) funded by the Ministry of Science. Z.L. acknowledges the support from RIE2020 AME Programmatic Grant funded by A*STAR-SERC, Singapore (Grant No. A18A1b0045). X.G. acknowledges funding support through the Shanghai Science and Technology Commission (grant no. 19JC1412400), the National Science Fund for Excellent Young Scholars (grant no. 61922057). C.D. acknowledges National Science Foundation CAREER: Conformable Piezoelectrics for Soft Tissue Imaging (grant no. 2044688) and MIT Media Lab Consortium funding. D.K. and O.G.S. acknowledge Leibniz Association and the German Research Foundation DFG (Gottfried Wilhelm Leibniz Program SCHM 1298/22-1, KA5051/1-1 and KA 5051/3-1), as well as the Leibniz association (Leibniz Transfer Program T62/2019). C.W. acknowledges the National Key Research and Development Program of China (grant no. 2021YFA1202600), National Natural Science Foundation of China (grant no. 62174082). A.V.-Y.T., E.Z., Y.Z., X.Z., and J.P. acknowledge the National Research Foundation, Singapore (NRF) under NRF’s Medium Sized Centre: Singapore Hybrid-Integrated Next-Generation μElectronics (SHINE) Centre funding programme, and AME programming funding scheme of Cyber Physiochemical Interface (CPI) project (no. A18A1b0045). R.Z. acknowledges National Natural Science Foundation of China (grant no. 51735007) and Beijing Natural Science Foundation (grant no. 3191001). N.M. acknowledges the support by JST PRESTO Grant Number JPMJPR20B7 and JST Adaptable and Seamless Technology transfer Program through Target-driven R&D (ASTEP) grant number JPMJTM22BK. C.P. acknowledges the Korean government (Ministry of Science and ICT, MSIT) (2022R1A4A3032923). M.W. acknowledges the National Key R&D Program of China under Grant (2021YFB3601200). X.Z. acknowledges National Natural Science Foundation of China (no. 62074029). S.X. acknowledges the 3M nontenured faculty award. T.-W.L. and D.-G.S. acknowledge the Pioneer Research Center Program through the National Research Foundation of Korea funded by the Ministry of Science, ICT & Future Planning (grant no. NRF-2022M3C1A3081211). C.T.L. would like to acknowledge support from the Institute for Health Innovation and Technology (iHealthtech), the MechanoBioEngineering Laboratory at the Department of Biomedical Engineering and the Institute for Functional Intelligent Materials (I-FIM) at the National University of Singapore (NUS). C.T.L. also acknowledges support from the National Research Foundation and A*STAR, under its RIE2020 Industry Alignment Fund − Industry Collaboration Projects (IAF-ICP) (grant no. I2001E0059) − SIA-NUS Digital Aviation Corp Lab and the NUS ARTIC Research (grant no. HFM-RP1). X.Y. acknowledges funding support by City University of Hong Kong (grant no. 9667221). T.X. and X.Z. acknowledge National Natural Science Foundation of China (22234006). B.C.K.T. acknowledges Cyber-Physiochemical Interfaces CPI, A*STAR A18A1b0045. H.G. acknowledges a research start-up grant (002479-00001) from Nanyang Technological University and the Agency for Science, Technology and Research (A*STAR) in Singapore. W.G. acknowledges National Science Foundation grant 2145802. D.J.L. acknowledges support from the US National Science Foundation grant number CBET-2223566. G.Y. acknowledges support from The Welch Foundation award F-1861, and Camille Dreyfus Teacher-Scholar Award. M.D.D. acknowledges funding support from NSF (grant no. EEC1160483). J.-H.A acknowledges the National Research Foundation of Korea (NRF-2015R1A3A2066337). J.C. acknowledges the Henry Samueli School of Engineering & Applied Science and the Department of Bioengineering at the University of California, Los Angeles for startup support and a Brain & Behavior Research Foundation Young Investigator Grant. K.T. acknowledges JST AIP Accelerated Program (no. JPMJCR21U1) and JSPS KAKENHI (grant no. JP22H00594). P.S.W. acknowledges the National Science Foundation (CMMI1636136) for support. A.M.A., M.C.H., and P.S.W. thank the National Institute on Drug Abuse (DA045550) for support. S.M. and X.C. appreciated the support from the Smart Grippers for Soft Robotics (SGSR) Programme under the National Research Foundation, Prime Minister’s Office, Singapore under its Campus of Research Excellence and Technological Enterprise (CREATE) programme.

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.

For the last decade, researchers have studied the creation of self-healable polymeric materials with desired properties for advanced applications. Since the polymeric network governs the overall behavior, precise control over the polymer morphology is important. Among the controlling strategies, the chemical structure of dynamic stickers in polymer chains can determine the polymer networks, which directly affect the macroscopic properties. However, it has been rarely understood how the sticker structure determines the polymer properties. Here, we systematically modulated dynamic mechanical responses of the polymer networks by adjusting the angles that a single sticker unit makes. From this study, we found that the polymer with periodic 180° stickers stacks well and forms a strong network, while the polymer with 120° stickers is twisted and forms a vulnerable network. Therefore, the 180° stickers induce high toughness and non-self-healable properties. On the other hand, polymers with 120° stickers are soft but easily self-healed. Finally, we mixed these two different angled stickers to have both mechanically tough and self-healable properties. This study of an angular factor in polymeric materials will be an important consideration for future materials for achieving superior properties.

An elastic printed circuit board (E-PCB) is a conductive framework used for the facile assembly of system-level stretchable electronics. E-PCBs require elastic conductors that have high conductivity, high stretchability, tough adhesion to various components, and imperceptible resistance changes even under large strain. We present a liquid metal particle network (LMP Net ) assembled by applying an acoustic field to a solid-state insulating liquid metal particle composite as the elastic conductor. The LMP Net conductor satisfies all the aforementioned requirements and enables the fabrication of a multilayered high-density E-PCB, in which numerous electronic components are intimately integrated to create highly stretchable skin electronics. Furthermore, we could generate the LMP Net in various polymer matrices, including hydrogels, self-healing elastomers, and photoresists, thus showing their potential for use in soft electronics.

Feeling temperature and touch The range of receptors in our skin make it possible to sense when we are touching an object and also gives us a general sense of the temperature of that object. Achieving this in an artificial skin-like material has been a challenge because most of the approaches for sensing touch are themselves temperature sensitive. You et al. studied the ion relaxation dynamics in a conductive elastomeric film (see the Perspective by Liu). They show that the ion relaxation time can be used as a strain-insensitive intrinsic variable for detecting temperature and the capacitance can be used as a temperature-insensitive extrinsic variable for sensing the strain, thus decoupling the two so that their signals do not interfere with each other. Science , this issue p. 961 ; see also p. 910

Polymeric materials in nature regularly employ ordered, hierarchical structures in order to perform unique and precise functions. Importantly, these structures are often formed and stabilized by the cooperative summation of many weak interactions as opposed to the independent association of a few strong bonds. Here, we show that synthetic, flexible polymer chains with periodically placed and directional dynamic bonds collectively assemble into supramolecular nanofibers when the overall molecular weight is below the polymer's critical entanglement molecular weight. This causes bulk films of long polymer chains to have faster dynamics than films of shorter polymer chains of identical chemical composition. The formation of nanofibers increases the bulk film modulus by over an order of magnitude and delays the onset of terminal flow by more than 100 °C, while still remaining solution processable. Systematic investigation of different polymer chain architectures and dynamic bonding moieties along with coarse-grained molecular dynamics simulations illuminate governing structure-function relationships that determine a polymer's capacity to form supramolecular nanofibers. This report of the cooperative assembly of multivalent polymer chains into hierarchical, supramolecular structures contributes to our fundamental understanding of designing biomimetic functional materials.

We present a comprehensive investigation of mechanical properties of supramolecular polymer networks with rationally developed multistrength hydrogen-bonding interactions. Self-healing poly(dimethy...

Conjugation breakers (CBs) with different H-bonding chemistries and linker flexibilities are designed and incorporated into a diketopyrrolopyrrole (DPP)-based conjugated polymer backbone. The effects of H-bonding interactions on polymer semiconductor morphology, mechanical properties, and electrical performance are systematically investigated. We observe that CBs with an H-bonding self-association constant >0.7 or a denser packing tendency are able to induce higher polymer chain aggregation and crystallinity in as-casted thin films, resulting in a higher modulus and crack on-set strain. Additionally, the rDoC (relative degree of crystallinity) of the stretched thin film with the highest crack on-set strain only suffers a small decrease, suggesting the main energy dissipation mechanism is the breakage of H-bonding interactions. By contrast, other less stretchable polymer films dissipate strain energy through the breakage of crystalline domains, indicated by a drastic decrease in rDoC. Furthermore, we evaluate their electrical performances under mechanical strain in fully stretchable field-effect transistors. The polymer with the highest crack on-set strain has the least degradation in mobility as a function of strain. Overall, these observations suggest that we can aptly tune the mechanical properties of a polymer semiconductor by modulating intermolecular interactions, such as H-bonding chemistry and linker flexibility. Such understanding provides molecular design guidelines for future stretchable semiconductors.

Artificial muscles are indispensable components for next-generation robotics capable of mimicking sophisticated movements of living systems. However, an optimal combination of actuation parameters, including strain, stress, energy density and high mechanical strength, is required for their practical applications. Here we report mammalian-skeletal-muscle-inspired single fibres and bundles with large and strong contractive actuation. The use of exfoliated graphene fillers within a uniaxial liquid crystalline matrix enables photothermal actuation with large work capacity and rapid response. Moreover, the reversible percolation of graphene fillers induced by the thermodynamic conformational transition of mesoscale structures can be in situ monitored by electrical switching. Such a dynamic percolation behaviour effectively strengthens the mechanical properties of the actuator fibres, particularly in the contracted actuation state, enabling mammalian-muscle-like reliable reversible actuation. Taking advantage of a mechanically compliant fibre structure, smart actuators are readily integrated into strong bundles as well as high-power soft robotics with light-driven remote control.

Semiconducting polymer thin films are essential elements of soft electronics for both wearable and biomedical applications

The authors have requested that this preprint be removed from Research Square.

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.

Shape memory polymers are promising materials in many emerging applications due to their large extensibility and excellent shape recovery. However, practical application of these polymers is limited by their poor energy densities (up to ∼1 MJ/m3). Here, we report an approach to achieve a high energy density, one-way shape memory polymer based on the formation of strain-induced supramolecular nanostructures. As polymer chains align during strain, strong directional dynamic bonds form, creating stable supramolecular nanostructures and trapping stretched chains in a highly elongated state. Upon heating, the dynamic bonds break, and stretched chains contract to their initial disordered state. This mechanism stores large amounts of entropic energy (as high as 19.6 MJ/m3 or 17.9 J/g), almost six times higher than the best previously reported shape memory polymers while maintaining near 100% shape recovery and fixity. The reported phenomenon of strain-induced supramolecular structures offers a new approach toward achieving high energy density shape memory polymers., We report an approach to achieve a high energy density shape memory polymer based on the formation of strain-induced supramolecular nanostructures, which immobilize stretched chains to store entropic energy.

Summary Implementation of lithium (Li)-metal anodes requires developments to solve the heterogeneity and instability issues of naturally formed solid-electrolyte interphase (SEI). The artificial SEI, as an alternative, enables an ideal interface by regulating critical features such as fast ion transport, conformal protection, and parasitic reaction mitigation. Herein, for the first time, we integrate all of these desired properties into a single matrix, the dynamic single-ion-conductive network (DSN), as a multifunctional artificial SEI. The DSN incorporates the tetrahedral Al(OR)4− (R = soft fluorinated linker) centers as both dynamic bonding motifs and counter anions, endowing it with flowability and Li+ single-ion conductivity. Simultaneously, the fluorinated linkers provide chain mobility and electrolyte-blocking capability. A solution-processed DSN coating was found to simultaneously hinder electrolyte penetration, mitigate side reactions between Li and electrolyte, maintain low interfacial impedance, and allow homogenous Li deposition. With this coating, long cycle life and high Coulombic efficiency are achieved for Li-metal battery in a commercial carbonate electrolyte.

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.

By relaying neural signals from the motor cortex to muscles, devices for neurorehabilitation can enhance the movement of limbs in which nerves have been damaged as a consequence of injuries affecting the spinal cord or the lower motor neurons. However, conventional neuroprosthetic devices are rigid and power-hungry. Here we report a stretchable neuromorphic implant that restores coordinated and smooth motions in the legs of mice with neurological motor disorders, enabling the animals to kick a ball, walk or run. The neuromorphic implant acts as an artificial efferent nerve by generating electrophysiological signals from excitatory post-synaptic signals and by providing proprioceptive feedback. The device operates at low power (~1/150 that of a typical microprocessor system), and consists of hydrogel electrodes connected to a stretchable transistor incorporating an organic semiconducting nanowire (acting as an artificial synapse), connected via an ion gel to an artificial proprioceptor incorporating a carbon nanotube strain sensor (acting as an artificial muscle spindle). Stretchable electronics with proprioceptive feedback may inspire the further development of advanced neuromorphic devices for neurorehabilitation.

Bioelectronics for modulating the nervous system have shown promise in treating neurological diseases(1–3). However, their fixed dimensions cannot accommodate rapid tissue growth(4,5) and may impair development(6). For infants, children and adolescents, once implanted devices are outgrown, additional surgeries are often needed for device replacement, leading to repeated interventions and complications(6–8). Here, we address this limitation with morphing electronics, which adapt to in vivo nerve tissue growth with minimal mechanical constraint. We design and fabricate multilayered morphing electronics, consisting of viscoplastic electrodes and a strain sensor that eliminate the stress at the interface between the electronics and growing tissue. The ability of morphing electronics to self-heal during implantation surgery allows a reconfigurable and seamless neural interface. During the fastest growth period in rats, morphing electronics caused minimal damage to the rat nerve, which grows 2.4-fold in diameter, and allowed chronic electrical stimulation and monitoring for 2 months without disruption of functional behavior. Morphing electronics offers a path toward growth-adaptive pediatric electronic medicine.

The cross-linking of conjugated polymers has been demonstrated to be an effective strategy to improve its elastic properties to give deformable semiconductors for plastic electronics. While there have been extensive studies of the structural requirements of the polymer host for good film ductility, no work to date has focused on the relevance of the structural design or chemistry of these cross-linker additives. In this study, urethane groups and tertiary carbon atoms are inserted into the alkyl backbone of perfluorophenyl azide-based cross-linkers to investigate the importance of cross-linker crystallinity with respect to polymer morphology and hence mechanical and electrical properties. Linear cross-linkers with hydrogen bonding from urethane groups readily phase separate and recrystallize in the polymer network to form cross-linked domains that obstruct the strain distribution of the polymer film. Branch cross-linkers with tertiary carbon on the other hand form an evenly cross-linked network in the pol...

I've got a feeling Sensory (or afferent) nerves bring sensations of touch, pain, or temperature variation to the central nervous system and brain. Using the tools and materials of organic electronics, Kim et al. combined a pressure sensor, a ring oscillator, and an ion gel–gated transistor to form an artificial mechanoreceptor (see the Perspective by Bartolozzi). The combination allows for the sensing of multiple pressure inputs, which can be converted into a sensor signal and used to drive the motion of a cockroach leg in an oscillatory pattern. Science , this issue p. 998 ; see also p. 966

Molecular additives are often used to enhance dynamic motion of polymeric chains, which subsequently alter the functional and physical properties of polymers. However, controlling the chain dynamics of semiconducting polymer thin films and understanding the fundamental mechanisms of such changes is a new area of research. Here, cycloparaphenylenes (CPPs) are used as conjugated molecular additives to tune the dynamic behaviors of diketopyrrolopyrrole-based (DPP-based) semiconducting polymers. It is observed that the addition of CPPs results in significant improvement in the stretchability of the DPP-based polymers without adversely affecting their mobility, which arises from the enhanced polymer dynamic motion and reduced long-range crystalline order. The polymer films retain their fiber-like morphology and short-range ordered aggregates, which leads to high mobility. Fully stretchable transistors are subsequently fabricated using CPP/semiconductor composites as active layers. These composites are observed to maintain high mobilities when strained and after repeated applied strains. Interestingly, CPPs are also observed to improve the contact resistance and charge transport of the fully stretchable transistors. ln summary, these results collectively indicate that controlling the dynamic motion of polymer semiconductors is proved to be an effective way to improve their stretchability.

Both self-healable conductors and stretchable conductors have been previously reported. However, it is still difficult to simultaneously achieve high stretchability, high conductivity, and self-healability. Here, we observed an intriguing phenomenon, termed “electrical self-boosting”, which enables reconstructing of electrically percolative pathways in an ultrastretchable and self-healable nanocomposite conductor (over 1700% strain). The autonomously reconstructed percolative pathways were directly verified by using microcomputed tomography and in situ scanning electron microscopy. The encapsulated nanocomposite conductor shows exceptional conductivity (average value: 2578 S cm–1; highest value: 3086 S cm–1) at 3500% tensile strain by virtue of efficient strain energy dissipation of the self-healing polymer and self-alignment and rearrangement of silver flakes surrounded by spontaneously formed silver nanoparticles and their self-assembly in the strained self-healing polymer matrix. In addition, the condu...

High‐transconductance stretchable transistors are important for conformable and sensitive sensors for wearables and soft robotics. Remarkably high transconductance, which enables large amplification of signals, has been achieved through the use of organic electrochemical transistors (OECTs). However, the stretchability of such systems has been tempered by the lack of stretchable conductors with high stability in electrolytes, high conductance at high strain (100%), and process compatibility with active layers. Highly stretchable and strain‐resistant Au conductors employed to fabricate intrinsically stretchable OECTs are demonstrated. Notably, the conductors exhibit a sheet resistance of 33.3 Ω Sq.−1 at 120% strain, the lowest reported value to date among stretchable Au thin film conductors. High‐performance stretchable Au is realized by suppressing strain‐induced microcrack propagation through control of the microcracks formed in deposited Au thin films. Then, the highly stretchable Au conductors are utilized to fabricate intrinsically stretchable OECTs with a high transconductance both at 0% strain (0.54 mS) and 140% strain (0.14 mS). Among previously reported systems, these OECTs show the highest transconductance at high strain (>50%). Finally, the high‐performance OECTs are utilized in stretchable synaptic transistors, which are critically important for the development of soft neuromorphic computing systems to provide artificial intelligence for future soft robotics. NRF (Natl Research Foundation, S’pore) ASTAR (Agency for Sci., Tech. and Research, S’pore) MOE (Min. of Education, S’pore) Accepted version

We developed a stretchable organic optoelectronic sensorimotor synapse to mimic a biological optical sensory nervous system., Emulation of human sensory and motor functions becomes a core technology in bioinspired electronics for next-generation electronic prosthetics and neurologically inspired robotics. An electronic synapse functionalized with an artificial sensory receptor and an artificial motor unit can be a fundamental element of bioinspired soft electronics. Here, we report an organic optoelectronic sensorimotor synapse that uses an organic optoelectronic synapse and a neuromuscular system based on a stretchable organic nanowire synaptic transistor (s-ONWST). The voltage pulses of a self-powered photodetector triggered by optical signals drive the s-ONWST, and resultant informative synaptic outputs are used not only for optical wireless communication of human-machine interfaces but also for light-interactive actuation of an artificial muscle actuator in the same way that a biological muscle fiber contracts. Our organic optoelectronic sensorimotor synapse suggests a promising strategy toward developing bioinspired soft electronics, neurologically inspired robotics, and electronic prostheses.

Skin-inspired semiconductor that is intrinsically stretchable, self-healable, and strain-sensitive for advanced sensory devices., Skin-like sensory devices should be stretchable and self-healable to meet the demands for future electronic skin applications. Despite recent notable advances in skin-inspired electronic materials, it remains challenging to confer these desired functionalities to an active semiconductor. Here, we report a strain-sensitive, stretchable, and autonomously self-healable semiconducting film achieved through blending of a polymer semiconductor and a self-healable elastomer, both of which are dynamically cross-linked by metal coordination. We observed that by controlling the percolation threshold of the polymer semiconductor, the blend film became strain sensitive, with a gauge factor of 5.75 × 105 at 100% strain in a stretchable transistor. The blend film is also highly stretchable (fracture strain, >1300%) and autonomously self-healable at room temperature. We proceed to demonstrate a fully integrated 5 × 5 stretchable active-matrix transistor sensor array capable of detecting strain distribution through surface deformation.

Popping open one by one into polymers We rarely board airplanes by joining the back of a single well-ordered line. More often, we jostle around in one of several bulging crowds that merge haphazardly near the gate. Roughly speaking, these processes are analogous to the chain growth and step growth mechanisms of polymer assembly at the molecular level. Kang et al. present a strategy to link molecular building blocks through hydrogen bonding in accord with the well-controlled chain growth model. The molecules start out curled inward, as they engage in internal hydrogen bonding, until an initiator pulls one open; that molecule is then in the right conformation to pull a partner into the growing chain, poising it to pull in yet another, and so forth down the line. Science , this issue p. 646

Because of a rapid conformational inversion, bowl-shaped C5-symmetric corannulenes, though geometrically chiral, have not been directly resolved into their enantiomers. However, if this inversion equilibrium can be desymmetrized, chiral corannulenes enriched in either enantiomer can be obtained. We demonstrated this possibility using pentasubstituted corannulenes 4 and 5 carrying amide-appended thioalkyl side chains. Compound 4 displays chiroptical activity in a chiral hydrocarbon such as limonene. Because compound 5 carries a chiral center in the side chains, its enantiomers 5R and 5S show chiroptical activity even in achiral solvents such as CHCl3 and methylcyclohexane. In sharp contrast, when the side chains bear no amide functionality (1 and 2R), no chiroptical activity emerges even in limonene or with a chiral center in the side chains. Detailed investigations revealed that the peripheral amide units in 4 and 5 are hydrogen-bonded only “intramolecularly” along the corannulene periphery, affording cyc...

This work was supported by Air Force Office of Scientific Research (Grant No. FA9550-18-1-0143) for financial support. M.N. acknowledges financial support from the European Commission through a Marie-Curie Individual Fellowship (EC Grant Agreement Number: 747461). H.T. was supported by an appointment to the Intelligence Community Postdoctoral Research Fellowship Program at Stanford University, administered by Oak Ridge Institute for Science and Education through an interagency agreement between the U.S. Department of Energy and the Office of the Director of National Intelligence. S.Z. and X.G. thank the financial support from U.S. Department of Energy, Office of Science, Office of Basic Energy Science under award number DE-SC0019361 and National Science Foundation Office of Integrative Activities #1757220. J.M. acknowledges Samsung Scholarship for financial support. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under award ECCS-1542152. GIXD measurement was carried out at the Stanford Synchrotron Radiation Laboratory (SSRL), a national user facility operated by Stanford University on behalf of the U.S. Department of Energy, Office of Basic Energy Sciences.

An electronic (e-) skin is expected to experience significant wear and tear over time. Therefore, self-healing stretchable materials that are simultaneously soft and with high fracture energy, that is high tolerance of damage or small cracks without propagating, are essential requirements for the realization of robust e-skin. However, previously reported elastomers and especially self-healing polymers are mostly viscoelastic and lack high mechanical toughness. Here, a new class of polymeric material crosslinked through rationally designed multistrength hydrogen bonding interactions is reported. The resultant supramolecular network in polymer film realizes exceptional mechanical properties such as notch-insensitive high stretchability (1200%), high toughness of 12 000 J m-2 , and autonomous self-healing even in artificial sweat. The tough self-healing materials enable the wafer-scale fabrication of robust and stretchable self-healing e-skin devices, which will provide new directions for future soft robotics and skin prosthetics.

Deformable electronic devices that are impervious to mechanical influence when mounted on surfaces of dynamically changing soft matters have great potential for next-generation implantable bioelectronic devices. Here, deformable field-effect transistors (FETs) composed of single organic nanowires (NWs) as the semiconductor are presented. The NWs are composed of fused thiophene diketopyrrolopyrrole based polymer semiconductor and high-molecular-weight polyethylene oxide as both the molecular binder and deformability enhancer. The obtained transistors show high field-effect mobility >8 cm2 V-1 s-1 with poly(vinylidenefluoride-co-trifluoroethylene) polymer dielectric and can easily be deformed by applied strains (both 100% tensile and compressive strains). The electrical reliability and mechanical durability of the NWs can be significantly enhanced by forming serpentine-like structures of the NWs. Remarkably, the fully deformable NW FETs withstand 3D volume changes (>1700% and reverting back to original state) of a rubber balloon with constant current output, on the surface of which it is attached. The deformable transistors can robustly operate without noticeable degradation on a mechanically dynamic soft matter surface, e.g., a pulsating balloon (pulse rate: 40 min-1 (0.67 Hz) and 40% volume expansion) that mimics a beating heart, which underscores its potential for future biomedical applications.

While encouraging progress has been made on switchable nanopores to mimic biological channels and pores, it remains a great challenge to realize long tubular pores with a dynamic open–closed motion. Here we report μm-long, dynamic tubular pores that undergo rapid switching between open and closed states in response to a thermal signal in water. The tubular walls consist of laterally associated primary fibrils stacked from disc-shaped molecules in which the discs readily tilt by means of thermally regulated dehydration of the oligoether chains placed on the wall surfaces. Notably, this pore switching mediates a controlled water-pumping catalytic action for the dehydrative cyclization of adenosine monophosphate to produce metabolically active cyclic adenosine monophosphate. We believe that our work may allow the creation of a variety of dynamic pore structures with complex functions arising from open–closed motion., Synthetic switchable nanopores may be useful for mimicking biological processes. Here, the authors report dynamic tubular pores that undergo rapid switching between open and closed states in response to a thermal signal in water and which can mediate a controlled water-pumping catalytic action.

Over the past decade, major progress in supramolecular polymerization has had a substantial effect on the design of functional soft materials. However, despite recent advances, most studies are still based on a preconceived notion that supramolecular polymerization follows a step-growth mechanism, which precludes control over chain length, sequence, and stereochemical structure. Here we report the realization of chain-growth polymerization by designing metastable monomers with a shape-promoted intramolecular hydrogen-bonding network. The monomers are conformationally restricted from spontaneous polymerization at ambient temperatures but begin to polymerize with characteristics typical of a living mechanism upon mixing with tailored initiators. The chain growth occurs stereoselectively and therefore enables optical resolution of a racemic monomer.

Because of a rapid conformational inversion, bowl-shaped C5-symmetric corannulenes, though geometrically chiral, have not been directly resolved into their enantiomers. However, if this inversion equilibrium can be desymmetrized, chiral corannulenes enriched in either enantiomer can be obtained. We demonstrated this possibility using pentasubstituted corannulenes 4 and 5 carrying amide-appended thioalkyl side chains. Compound 4 displays chiroptical activity in a chiral hydrocarbon such as limonene. Because compound 5 carries a chiral center in the side chains, its enantiomers 5R and 5S show chiroptical activity even in achiral solvents such as CHCl3 and methylcyclohexane. In sharp contrast, when the side chains bear no amide functionality (1 and 2R), no chiroptical activity emerges even in limonene or with a chiral center in the side chains. Detailed investigations revealed that the peripheral amide units in 4 and 5 are hydrogen-bonded only "intramolecularly" along the corannulene periphery, affording cyclic amide networks with clockwise and anticlockwise geometries. Although this networking gives rise to four stereoisomers, only two, which are enantiomeric to one another, are suggested computationally to exist in the equilibrated system. In a chiral environment (chiral solvent or side chain), their thermodynamic stabilities are certainly unequal, so the bowl-inversion equilibrium can be desymmetrized. However, this is not the case when the system contains a protic solvent that can deteriorate the hydrogen-bonding network. When the enantiomeric purity of limonene as the solvent is varied, the chiroptical activity of the corannulene core changes nonlinearly with its enantiomeric excess (majority rule).