Observing Proton-Electron Mixed Conductivity in Graphdiyne.

Mixed conducting materials with both ionic and electronic conductivities have gained prominence in emerging applications. However, exploring material with on-demand ionic and electronic conductivities remains challenging, primarily due to the lack of correlating macroscopic conductivity with atom-scale structure. Here, the correlation of proton-electron conductivity and atom-scale structure in graphdiyne is explored. Precisely adjusting the conjugated diynes and oxygenic functional groups in graphdiyne yields a tunable proton-electron conductivity on the order of 103. In addition, a wet-chemistry lithography technique for uniform preparation of graphdiyne on flexible substrates is provided. Utilizing the proton-electron conductivity and mechanical tolerance of graphdiyne, bimodal flexible devices serving as capacitive switches and resistive sensors are created. As a proof-of-concept, a breath-machine interface for sentence-based communication and self-nursing tasks with an accuracy of 98% is designed. This work represents an important step toward understanding the atom-scale structure-conductivity relationship and extending the applications of mixed conducting materials to assistive technology.

Bioinspired Double-Broadband Switchable Microwave Absorbing Grid Structures with Inflatable Kresling Origami Actuators.

Tunable radar stealth structures are critical components for future military equipment because of their potential to further enhance the design space and performance. Some previous investigations have utilized simple origami structures as the basic adjusting components but failed to achieve the desired broadband microwave absorbing characteristic. Herein, a novel double-broadband switchable microwave absorbing grid structure has been developed with the actuators of inflatable Kresling origami structures. Geometric constraints are derived to endow a bistable feature with this origami configuration, and the stable states are switched by adjusting the internal pressure. An ultra-broadband microwave absorbing structure is proposed with a couple of complementary microwave stealth bands, and optimized by a particle swarm optimization algorithm. The superior electromagnetic performance results from the mode switch activating different absorbing components at corresponding frequencies. A digital adjusting strategy is applied, which effectively achieves a continuously adjusting effect. Further investigations show that the proposed structure possesses superior robustness. In addition, minimal interactions are found between adjacent grid units, and the electromagnetic performance is mainly related to the duty ratio of the units in different states. They have enhanced the microwave absorbing performance of grid structures through a tunable design, a provided a feasible paradigm for other tunable absorbers.

Water-responsive supercontractile polymer films for bioelectronic interfaces.

Connecting different electronic devices is usually straightforward because they have paired, standardized interfaces, in which the shapes and sizes match each other perfectly. Tissue-electronics interfaces, however, cannot be standardized, because tissues are soft1-3 and have arbitrary shapes and sizes4-6. Shape-adaptive wrapping and covering around irregularly sized and shaped objects have been achieved using heat-shrink films because they can contract largely and rapidly when heated7. However, these materials are unsuitable for biological applications because they are usually much harder than tissues and contract at temperatures higher than 90 °C (refs. 8,9). Therefore, it is challenging to prepare stimuli-responsive films with large and rapid contractions for which the stimuli and mechanical properties are compatible with vulnerable tissues and electronic integration processes. Here, inspired by spider silk10-12, we designed water-responsive supercontractile polymer films composed of poly(ethylene oxide) and poly(ethylene glycol)-α-cyclodextrin inclusion complex, which are initially dry, flexible and stable under ambient conditions, contract by more than 50% of their original length within seconds (about 30% per second) after wetting and become soft (about 100 kPa) and stretchable (around 600%) hydrogel thin films thereafter. This supercontraction is attributed to the aligned microporous hierarchical structures of the films, which also facilitate electronic integration. We used this film to fabricate shape-adaptive electrode arrays that simplify the implantation procedure through supercontraction and conformally wrap around nerves, muscles and hearts of different sizes when wetted for in vivo nerve stimulation and electrophysiological signal recording. This study demonstrates that this water-responsive material can play an important part in shaping the next-generation tissue-electronics interfaces as well as broadening the biomedical application of shape-adaptive materials.

Contact Lens Sensor with Anti-jamming Capability and High Sensitivity for Intraocular Pressure Monitoring.

Contact lens sensors provide a noninvasive approach for intraocular pressure (IOP) monitoring in patients with glaucoma. Accurate measurement of this imperceptible pressure variation requires highly sensitive sensors in the absence of simultaneously amplifying IOP signal and blinking-induced noise. However, current noise-reduction methods rely on external filter circuits, which thicken contact lenses and reduce signal quality. Here, we introduce a contact lens strain sensor with an anti-jamming ability by utilizing a self-lubricating layer to reduce the coefficient of friction (COF) to remove the interference from the tangential force. The sensor achieves exceptionally high sensitivity due to the strain concentration layout and the confined occurrence of sympatric microcracks. The animal tests prove our lens can accurately detect IOP safely and reliably.

Conductive Metal-Organic Frameworks with Tunable Dielectric Properties for Boosting Electromagnetic Wave Absorption.

Metal-organic frameworks (MOFs) manifest enormous potential in promoting electromagnetic wave (EMW) absorption thanks to the tailored components, topological structure, and high porosity. Herein, rodlike conductive MOFs (cMOFs) composed of adjustable metal ions of Zn, Cu, Co, or Ni and ligands of hexahydroxytriphenylene (HHTP) are prepared to attain tunable dielectric properties for a tailored EMW absorption. Specifically, the influences of the cMOFs' composition, charge transport characteristic, topological crystalline structure, and anisotropy microstructure on dielectric and EMW absorption performance are ascertained, advancing the understanding of EMW attenuation mechanisms of MOFs. The boosted conductive and polarization losses derived from the conjugation effects and terminal groups, as well as shape anisotropy, lead to a prominent EMW absorption of the cMOFs. The Cu-HHTP confers a minimum reflection loss (RLmin) of -63.55 dB at the thickness of 2.9 mm and a maximum effective absorption bandwidth of 5.2 GHz. Moreover, Zn-HHTP showcases the absorption superiority in the S-band (2-4 GHz) with an RLmin of -62.8 dB at a thickness of 1.9 mm. This work not only hoists the mechanistic understanding of the structure-function relationships for the cMOFs but also offers guidelines for preparing functional MOF materials.

Self-Closing Stretchable Cuff Electrodes for Peripheral Nerve Stimulation and Electromyographic Signal Recording.

The cuff electrode can be wrapped in the columnar or tubular biological tissue for physiological signal detection or stimulation regulation. The reliable and non-excessive interfaces between the electrode and complex tissue are critical. Here, we propose a self-closing stretchable cuff electrode, which is able to self-close onto the bundles of tissues after dropping water. The curliness is realized by the mechanical stress mismatch between different layers of the elastic substrate. The material of the substrate can be selected to match the modulus of the target tissue to achieve minimal constraint on the tissue. Moreover, the self-closing structure keeps the cuff electrode free from any extra mechanical locking structure. For in vivo testing, both sciatic nerve stimulation to drive muscles and electromyographic signal monitoring around a rat's extensor digitorum longus for 1 month prove that our proposed electrode conforms well to the curved surface of biological tissue.

A universal interface for plug-and-play assembly of stretchable devices.

Stretchable hybrid devices have enabled high-fidelity implantable1-3 and on-skin4-6 monitoring of physiological signals. These devices typically contain soft modules that match the mechanical requirements in humans7,8 and soft robots9,10, rigid modules containing Si-based microelectronics11,12 and protective encapsulation modules13,14. To make such a system mechanically compliant, the interconnects between the modules need to tolerate stress concentration that may limit their stretching and ultimately cause debonding failure15-17. Here, we report a universal interface that can reliably connect soft, rigid and encapsulation modules together to form robust and highly stretchable devices in a plug-and-play manner. The interface, consisting of interpenetrating polymer and metal nanostructures, connects modules by simply pressing without using pastes. Its formation is depicted by a biphasic network growth model. Soft-soft modules joined by this interface achieved 600% and 180% mechanical and electrical stretchability, respectively. Soft and rigid modules can also be electrically connected using the above interface. Encapsulation on soft modules with this interface is strongly adhesive with an interfacial toughness of 0.24 N mm-1. As a proof of concept, we use this interface to assemble stretchable devices for in vivo neuromodulation and on-skin electromyography, with high signal quality and mechanical resistance. We expect such a plug-and-play interface to simplify and accelerate the development of on-skin and implantable stretchable devices.

Ultrathin Cellulose Nanofiber Assisted Ambient-Pressure-Dried, Ultralight, Mechanically Robust, Multifunctional MXene Aerogels.

Ambient-pressure-dried (APD) preparation of transition metal carbide/nitrides (MXene) aerogels is highly desirable yet remains highly challenging. Here, ultrathin, high-strength-to-weight-ratio, renewable cellulose nanofibers (CNFs) are efficiently utilized to assist in the APD preparation of ultralight yet robust, highly conductive, large-area MXene-based aerogels via a facile, energy-efficient, eco-friendly, and scalable freezing-exchanging-drying approach. The strong interactions of large-aspect-ratio CNF and MXene as well as the biomimetic nacre-like microstructure induce high mechanical strength and stability to avoid the structure collapse of aerogels in the APD process. Abundant functional groups of CNFs facilitate the chemical crosslinking of MXene-based aerogels, significantly improving the hydrophobicity, water resistance, and even oxidation stability. The ultrathin, 1D nature of the CNF renders the minimal MXenes' interlayered gaps and numerous heterogeneous interfaces, yielding the excellent conductivity and electromagnetic interference (EMI) shielding performance of aerogels. The synergies of the MXene, CNF, and abundant pores efficiently improve the EMI shielding performance, photothermal conversion, and absorption of viscous crude oil. This work shows great promises of the APD, multifunctional MXene-based aerogels in electromagnetic protection or compatibility, thermal therapy, and oil-water separation applications.

Shape morphing of plastic films.

Three-dimensional (3D) architectures have qualitatively expanded the functions of materials and flexible electronics. However, current fabrication techniques for devices constrain their substrates to 2D geometries and current post-shape transformation strategies are limited to heterogenous or responsive materials and are not amenable to free-standing inert plastic films such as polyethylene terephthalate (PET) and polyimide (PI), which are vital substrates for flexible electronics. Here, we realize the shape morphing of homogeneous plastic films for various free-standing 3D frameworks from their 2D precursors by introducing a general strategy based on programming the plastic strain in films under peeling. By modulating the peeling parameters, previously inaccessible free-standing 3D geometries ranging from millimeter to micrometer were predicted theoretically and obtained experimentally. This strategy is applicable to most materials capable of plastic deformation, including polymers, metals, and composite materials, and can even enable 4D transformation with responsive plastic films. Enhanced performance of 3D circuits and piezoelectric systems demonstrates the enormous potential of peeling-induced shape morphing for 3D devices.

Printable Aligned Single-Walled Carbon Nanotube Film with Outstanding Thermal Conductivity and Electromagnetic Interference Shielding Performance.

Ultrathin, lightweight, and flexible aligned single-walled carbon nanotube (SWCNT) films are fabricated by a facile, environmentally friendly, and scalable printing methodology. The aligned pattern and outstanding intrinsic properties render "metal-like" thermal conductivity of the SWCNT films, as well as excellent mechanical strength, flexibility, and hydrophobicity. Further, the aligned cellular microstructure promotes the electromagnetic interference (EMI) shielding ability of the SWCNTs, leading to excellent shielding effectiveness (SE) of ~ 39 to 90 dB despite a density of only ~ 0.6 g cm-3 at thicknesses of merely 1.5-24 µm, respectively. An ultrahigh thickness-specific SE of 25 693 dB mm-1 and an unprecedented normalized specific SE of 428 222 dB cm2 g-1 are accomplished by the freestanding SWCNT films, significantly surpassing previously reported shielding materials. In addition to an EMI SE greater than 54 dB in an ultra-broadband frequency range of around 400 GHz, the films demonstrate excellent EMI shielding stability and reliability when subjected to mechanical deformation, chemical (acid/alkali/organic solvent) corrosion, and high-/low-temperature environments. The novel printed SWCNT films offer significant potential for practical applications in the aerospace, defense, precision components, and smart wearable electronics industries.

Freestanding and Scalable Force-Softness Bimodal Sensor Arrays for Haptic Body-Feature Identification.

Tactile technologies that can identify human body features are valuable in clinical diagnosis and human-machine interactions. Previously, cutting-edge tactile platforms have been able to identify structured non-living objects; however, identification of human body features remains challenging mainly because of the irregular contour and heterogeneous spatial distribution of softness. Here, freestanding and scalable tactile platforms of force-softness bimodal sensor arrays are developed, enabling tactile gloves to identify body features using machine-learning methods. The bimodal sensors are engineered by adding a protrusion on a piezoresistive pressure sensor, endowing the resistance signals with combined information of pressure and the softness of samples. The simple design enables 112 bimodal sensors to be integrated into a thin, conformal, and stretchable tactile glove, allowing the tactile information to be digitalized while hand skills are performed on the human body. The tactile glove shows high accuracy (98%) in identifying four body features of a real person, and four organ models (healthy and pathological) inside an abdominal simulator, demonstrating identification of body features of the bimodal tactile platforms and showing their potential use in future healthcare and robotics.

Strain-Driven Auto-Detachable Patterning of Flexible Electrodes.

Flexible electrodes that are multilayer, multimaterial, and conformal are pivotal for multifunctional wearable electronics. Traditional electronic circuits manufacturing requires substrate-supported transfer printing, which limits their multilayer integrity and device conformability on arbitrary surfaces. Herein, a "shrinkage-assisted patterning by evaporation" (SHAPE) method is reported, by employing evaporation-induced interfacial strain mismatch, to fabricate auto-detachable, freestanding, and patternable electrodes. The SHAPE method utilizes vacuum-filtration of polyaniline/bacterial cellulose (PANI/BC) ink through a masked filtration membrane to print high-resolution, patterned, and multilayer electrodes. The strong interlayer hydrogen bonding ensures robust multilayer integrity, while the controllable evaporative shrinking property of PANI/BC induces mismatch between the strains of the electrode and filtration membrane at the interface and thus autodetachment of electrodes. Notably, a 500-layer substrateless micro-supercapacitor fabricated using the SHAPE method exhibits an energy density of 350 mWh cm-2 at a power density of 40 mW cm-2 , 100 times higher than reported substrate-confined counterparts. Moreover, a digital circuit fabricated using the SHAPE method functions stably on a deformed glove, highlighting the broad wearable applications of the SHAPE method.

Sliding Cyclodextrin Molecules along Polymer Chains to Enhance the Stretchability of Conductive Composites.

The demand for stretchable electronics with a broader working range is increasing for wide application in wearable sensors and e-skin. However, stretchable conductors based on soft elastomers always exhibit low working range due to the inhomogeneous breakage of the conductive network when stretched. Here, a highly stretchable and self-healable conductor is reported by adopting polyrotaxane and disulfide bonds into the binding layer. The binding layer (PR-SS) builds the bridge between polymer substrates (PU-SS) and silver nanowires (AgNWs). The incorporation of sliding molecules endows the stretchable conductor with a long sensing range (190%) due to the energy dissipation derived from the sliding nature of polyrotaxanes, which is two times higher than the working range (93%) of conductors based on AP-SS without polyrotaxanes. Furthermore, the mechanism of sliding effect for the polyrotaxanes in the elastomers is investigated by SEM for morphological change of AgNWs, in situ small-angle x-ray scattering, as well as stress relaxation experiments. Finally, human-body-related sensing tests and a self-correction system in fitness are designed and demonstrated.

A Mechanically Interlocking Strategy Based on Conductive Microbridges for Stretchable Electronics.

Stretchable electronics incorporating critical sensing, data transmission, display and powering functionalities, is crucial to emerging wearable healthcare applications. To date, methods to achieve stretchability of individual functional devices have been extensively investigated. However, integration strategies of these stretchable devices to achieve all-stretchable systems are still under exploration, in which the reliable stretchable interconnection is a key element. Here, solderless stretchable interconnections based on mechanically interlocking microbridges are developed to realize the assembly of individual stretchable devices onto soft patternable circuits toward multifunctional all-stretchable platforms. This stretchable interconnection can effectively bridge interlayer conductivity with tight adhesion through both conductive microbridges and selectively distributed adhesive polymer. Consequently, enhanced stretchability up to a strain of 35% (R/R0  ≤ 5) is shown, compared with conventional solder-assisted connections which lose electrical conduction at a strain of less than 5% (R/R0  ≈ 30). As a proof of concept, a self-powered all-stretchable data-acquisition platform is fabricated by surface mounting a stretchable strain sensor and a supercapacitor onto a soft circuit through solderless interconnections. This solderless interconnecting strategy for surface-mountable devices can be utilized as a valuable technology for the integration of stretchable devices to achieve all-soft multifunctional systems.

Strain-Enabled Phase Transition of Periodic Metasurfaces.

Phase transitions are universal in solid-state matters, as well as in periodic electromagnetic metasurfaces-the photonic analogues of crystals. Although such transitions dictate the properties of active metasurfaces, universal ways to describe the structure transition of periodic metasurfaces have not yet been established. Here, the authors report the strain-enabled phase transition (or lattice deformation) of stretchable metasurfaces with the crystallographic description. They analytically and experimentally demonstrate the phase transition of plasmonic lattices between two arbitrary 2D Bravais lattices under certain strain configurations. The strain-induced symmetry lowering of the structures gives rise to optical anisotropy upon polarization, namely, linearly and circularly polarized dichroism. They further demonstrate the potential of phase transition in information decoding with applied strain. Interpreting the phase transition of metasurfaces from a standpoint of symmetry would accelerate the discovery of emergent properties, and provide a generalizable approach to designing active metasurfaces.

Mechanically Durable Memristor Arrays Based on a Discrete Structure Design.

Memristors constitute a promising functional component for information storage and in-memory computing in flexible and stretchable electronics including wearable devices, prosthetics, and soft robotics. Despite tremendous efforts made to adapt conventional rigid memristors to flexible and stretchable scenarios, stretchable and mechanical-damage-endurable memristors, which are critical for maintaining reliable functions under unexpected mechanical attack, have never been achieved. Here, the development of stretchable memristors with mechanical damage endurance based on a discrete structure design is reported. The memristors possess large stretchability (40%) and excellent deformability (half-fold), and retain stable performances under dynamic stretching and releasing. It is shown that the memristors maintain reliable functions and preserve information after extreme mechanical damage, including puncture (up to 100 times) and serious tearing situations (fully diagonally cut). The structural strategy offers new opportunities for next-generation stretchable memristors with mechanical damage endurance, which is vital to achieve reliable functions for flexible and stretchable electronics even in extreme and highly dynamic environments.

Haptically Quantifying Young's Modulus of Soft Materials Using a Self-Locked Stretchable Strain Sensor.

Simple and rapid Young's modulus measurements of soft materials adaptable to various scenarios are of general significance, and they require miniaturized measurement platforms with easy operation. Despite the advances made in portable and wearable approaches, acquiring and analyzing multiple or complicated signals necessitate tethered bulky components and careful preparation. Here, a new methodology based on a self-locked stretchable strain sensor to haptically quantify Young's modulus of soft materials (kPa-MPa) rapidly is reported. The method demonstrates a fingertip measurement platform, which endows a prosthetic finger with human-comparable haptic behaviors and skills on elasticity sensing without activity constraints. A universal strategy is offered toward ultraconvenient and high-efficient Young's modulus measurements with wide adaptability to various fields for unprecedented applications.

Pangolin-Inspired Stretchable, Microwave-Invisible Metascale.

Microwave-invisible devices are emerging as a valuable technology in various applications, including soft robotics, shape-morphing structures, and textural camouflages, especially in electronic countermeasures. Unfortunately, conventional microwave-absorbing metastructures and bulk absorbers are stretching confined, limiting their application in deformable or special-shaped targets. To overcome such limitations, a conceptually novel soft-rigid-connection strategy, inspired by the pangolin, is proposed. Pangolin-inspired metascale (PIMS), which is a kind of stretchable metamaterial consisting of an electromagnetic dissipative scale (EMD-scale) and elastomer, is rationally designed. Such a device exhibits robust microwave-absorbing capacity under the interference of 50% stretching. Besides, profiting from the covering effect and size-confined effect of EMD-scale, the out-of-plane indentation failure force of PIMS is at least 5 times larger than conventional device. As a proof of concept, the proposed device is conformally pasted on nondevelopable surfaces. For a spherical dome surface, the maximum radar cross-section (RCS) reduction of PIMS is 6.3 dB larger than that of a conventional device, while for a saddle surface, the bandwidth of 10 dB RCS reduction exhibits an increase of 83%. In short, this work provides a conceptually novel platform to develop stretchable, nondevelopable surface conformable functional devices.

Mechanomaterials: A Rational Deployment of Forces and Geometries in Programming Functional Materials.

The knowledge of mechanics of materials has been extensively implemented in developing functional materials, giving rise to recent advances in soft actuators, flexible electronics, mechanical metamaterials, tunable mechanochromics, regenerative mechanomedicine, etc. While conventional mechanics of materials offers passive access to mechanical properties of materials in existing forms, a paradigm shift is emerging toward proactive programming of materials' functionality by leveraging the force-geometry-property relationships. Here, such a rising field is coined as "mechanomaterials". To profile the concept, the design principles in this field at four scales is first outlined, namely the atomic scale, the molecular scale, the manipulation of nanoscale materials, and the microscale design of structural materials. A variety of techniques have been recruited to deliver the multiscale programming of functional mechanomaterials, such as strain engineering, capillary assembly, topological interlocking, kirigami, origami, to name a few. Engineering optical and biological functionalities have also been achieved by implementing the fundamentals of mechanochemistry and mechanobiology. Nonetheless, the field of mechanomaterials is still in its infancy, with many open challenges and opportunities that need to be addressed. The authors hope this review can serve as a modest spur to attract more researchers to further advance this field.

Highly Thermal-Wet Comfortable and Conformal Silk-Based Electrodes for On-Skin Sensors with Sweat Tolerance.

Noninvasive and seamless interfacing between the sensors and human skin is highly desired for wearable healthcare. Thin-film-based soft and stretchable sensors can to some extent form conformal contact with skin even under dynamic movements for high-fidelity signals acquisition. However, sweat accumulation underneath these sensors for long-term monitoring would compromise the thermal-wet comfort, electrode adherence to the skin, and signal fidelity. Here, we report the fabrication of a highly thermal-wet comfortable and conformal silk-based electrode, which can be used for on-skin electrophysiological measurement under sweaty conditions. It is realized through incorporating conducting polymers poly(3,4-ethylenedioxythiophene): polystyrenesulfonate (PEDOT:PSS) into glycerol-plasticized silk fiber mats. Glycerol plays the role of tuning the mechanical properties of silk fiber mats and enhancing the conductivity of PEDOT:PSS. Our silk-based electrodes show high stretchability (>250%), low thermal insulation (∼0.13 °C·m2·W-1), low evaporative resistance (∼23 Pa·m2·W-1, 10 times lower than ∼1.3 mm thick commercial gel electrodes), and high water-vapor transmission rate (∼117 g·m-2·h-1 under sweaty conditions, 2 times higher than skin water loss). These features enable a better electrocardiography signal quality than that of commercial gel electrodes without disturbing the heat dissipation during sweat evaporation and provide possibilities for textile integration to monitor the muscle activities under large deformation. Our glycerol-plasticized silk-based electrodes possessing superior physiological comfortability may further engage progress in on-skin electronics with sweat tolerance.