Highly Conductive and Stretchable Hydrogel Nanocomposite Using Whiskered Gold Nanosheets for Soft Bioelectronics.

The low electrical conductivity of conductive hydrogels limits their applications as soft conductors in bioelectronics. This low conductivity originates from the high water content of hydrogels, which impedes facile carrier transport between conductive fillers. This study presents a highly conductive and stretchable hydrogel nanocomposite comprising whiskered gold nanosheets. A dry network of whiskered gold nanosheets is fabricated and then incorporated into the wet hydrogel matrices. The whiskered gold nanosheets preserve their tight interconnection in hydrogels despite the high water content, providing a high-quality percolation network even under stretched states. Regardless of the type of hydrogel matrix, the gold-hydrogel nanocomposites exhibit a conductivity of ≈520 S cm-1 and a stretchability of ≈300% without requiring a dehydration process. The conductivity reaches a maximum of ≈3304 S cm-1 when the density of the dry gold network is controlled. A gold-adhesive hydrogel nanocomposite, which can achieve conformal adhesion to moving organ surfaces, is fabricated for bioelectronics demonstrations. The adhesive hydrogel electrode outperforms elastomer-based electrodes in in vivo epicardial electrogram recording, epicardial pacing, and sciatic nerve stimulation.

Electronic Skin: Opportunities and Challenges in Convergence with Machine Learning.

Recent advancements in soft electronic skin (e-skin) have led to the development of human-like devices that reproduce the skin's functions and physical attributes. These devices are being explored for applications in robotic prostheses as well as for collecting biopotentials for disease diagnosis and treatment, as exemplified by biomedical e-skins. More recently, machine learning (ML) has been utilized to enhance device control accuracy and data processing efficiency. The convergence of e-skin technologies with ML is promoting their translation into clinical practice, especially in healthcare. This review highlights the latest developments in ML-reinforced e-skin devices for robotic prostheses and biomedical instrumentations. We first describe technological breakthroughs in state-of-the-art e-skin devices, emphasizing technologies that achieve skin-like properties. We then introduce ML methods adopted for control optimization and pattern recognition, followed by practical applications that converge the two technologies. Lastly, we briefly discuss the challenges this interdisciplinary research encounters in its clinical and industrial transition.

Anti-distortion bioinspired camera with an inhomogeneous photo-pixel array.

The bioinspired camera, comprising a single lens and a curved image sensor-a photodiode array on a curved surface-, was born of flexible electronics. Its economical build lends itself well to space-constrained machine vision applications. The curved sensor, much akin to the retina, helps image focusing, but the curvature also creates a problem of image distortion, which can undermine machine vision tasks such as object recognition. Here we report an anti-distortion single-lens camera, where 4096 silicon photodiodes arrayed on a curved surface in a nonuniform pattern assimilated to the distorting optics are the key to anti-distortion engineering. That is, the photo-pixel distribution pattern itself is warped in the same manner as images are warped, which correctively reverses distortion. Acquired images feature no appreciable distortion across a 120° horizontal view, as confirmed by their neural-network recognition accuracies. This distortion correction via photo-pixel array reconfiguration is a form of in-sensor computing.

Needle-Like Multifunctional Biphasic Microfiber for Minimally Invasive Implantable Bioelectronics.

Implantable bioelectronics has attracted significant attention in electroceuticals and clinical medicine for precise diagnosis and efficient treatment of target diseases. However, conventional rigid implantable devices face challenges such as poor tissue-device interface and unavoidable tissue damage during surgical implantation. Despite continuous efforts to utilize various soft materials to address such issues, their practical applications remain limited. Here, a needle-like stretchable microfiber composed of a phase-convertible liquid metal (LM) core and a multifunctional nanocomposite shell for minimally invasive soft bioelectronics is reported. The sharp tapered microfiber can be stiffened by freezing akin to a conventional needle to penetrate soft tissue with minimal incision. Once implanted in vivo where the LM melts, unlike conventional stiff needles, it regains soft mechanical properties, which facilitate a seamless tissue-device interface. The nanocomposite incorporating with functional nanomaterials exhibits both low impedance and the ability to detect physiological pH, providing biosensing and stimulation capabilities. The fluidic LM embedded in the nanocomposite shell enables high stretchability and strain-insensitive electrical properties. This multifunctional biphasic microfiber conforms to the surfaces of the stomach, muscle, and heart, offering a promising approach for electrophysiological recording, pH sensing, electrical stimulation, and radiofrequency ablation in vivo.

Damage-free dry transfer method using stress engineering for high-performance flexible two- and three-dimensional electronics.

Advanced transfer printing technologies have enabled the fabrication of high-performance flexible and stretchable devices, revolutionizing many research fields including soft electronics, optoelectronics, bioelectronics and energy devices. Despite previous innovations, challenges remain, such as safety concerns due to toxic chemicals, the expensive equipment, film damage during the transfer process and difficulty in high-temperature processing. Thus a new transfer printing process is needed for the commercialization of high-performance soft electronic devices. Here we propose a damage-free dry transfer printing strategy based on stress control of the deposited thin films. First, stress-controlled metal bilayer films are deposited using direct current magnetron sputtering. Subsequently, mechanical bending is applied to facilitate the release of the metal bilayer by increasing the overall stress. Experimental and simulation studies elucidate the stress evolution mechanisms during the processes. By using this method, we successfully transfer metal thin films and high-temperature-treated oxide thin films onto flexible or stretchable substrates, enabling the fabrication of two-dimensional flexible electronic devices and three-dimensional multifunctional devices.

Stretchable Functional Nanocomposites for Soft Implantable Bioelectronics.

Material advances in soft bioelectronics, particularly those based on stretchable nanocomposites─functional nanomaterials embedded in viscoelastic polymers with irreversible or reversible bonds─have driven significant progress in translational medical device research. The unique mechanical properties inherent in the stretchable nanocomposites enable stiffness matching between tissue and device, as well as its spontaneous mechanical adaptation to in vivo environments, minimizing undesired mechanical stress and inflammation responses. Furthermore, these properties allow percolative networks of conducting fillers in the nanocomposites to be sustained even under repetitive tensile/compressive stresses, leading to stable tissue-device interfacing. Here, we present an in-depth review of materials strategies, fabrication/integration techniques, device designs, applications, and translational opportunities of nanocomposite-based soft bioelectronics, which feature intrinsic stretchability, self-healability, tissue adhesion, and/or syringe injectability. Among many, applications to brain, heart, and peripheral nerves are predominantly discussed, and translational studies in certain domains such as neuromuscular and cardiovascular engineering are particularly highlighted.

Next-Generation Cardiac Interfacing Technologies Using Nanomaterial-Based Soft Bioelectronics.

Cardiac interfacing devices are essential components for the management of cardiovascular diseases, particularly in terms of electrophysiological monitoring and implementation of therapies. However, conventional cardiac devices are typically composed of rigid and bulky materials and thus pose significant challenges for effective long-term interfacing with the curvilinear surface of a dynamically beating heart. In this regard, the recent development of intrinsically soft bioelectronic devices using nanocomposites, which are fabricated by blending conductive nanofillers in polymeric and elastomeric matrices, has shown great promise. The intrinsically soft bioelectronics not only endure the dynamic beating motion of the heart and maintain stable performance but also enable conformal, reliable, and large-area interfacing with the target cardiac tissue, allowing for high-quality electrophysiological mapping, feedback electrical stimulations, and even mechanical assistance. Here, we explore next-generation cardiac interfacing strategies based on soft bioelectronic devices that utilize elastic conductive nanocomposites. We first discuss the conventional cardiac devices used to manage cardiovascular diseases and explain their undesired limitations. Then, we introduce intrinsically soft polymeric materials and mechanical restraint devices utilizing soft polymeric materials. After the discussion of the fabrication and functionalization of conductive nanomaterials, the introduction of intrinsically soft bioelectronics using nanocomposites and their application to cardiac monitoring and feedback therapy follow. Finally, comments on the future prospects of soft bioelectronics for cardiac interfacing technologies are discussed.

Avian eye-inspired perovskite artificial vision system for foveated and multispectral imaging.

Avian eyes have deep central foveae as a result of extensive evolution. Deep foveae efficiently refract incident light, creating a magnified image of the target object and making it easier to track object motion. These features are essential for detecting and tracking remote objects in dynamic environments. Furthermore, avian eyes respond to a wide spectrum of light, including visible and ultraviolet light, allowing them to efficiently distinguish the target object from complex backgrounds. Despite notable advances in artificial vision systems that mimic animal vision, the exceptional object detection and targeting capabilities of avian eyes via foveated and multispectral imaging remain underexplored. Here, we present an artificial vision system that capitalizes on these aspects of avian vision. We introduce an artificial fovea and vertically stacked perovskite photodetector arrays whose designs were optimized by theoretical simulations for the demonstration of foveated and multispectral imaging. The artificial vision system successfully identifies colored and mixed-color objects and detects remote objects through foveated imaging. The potential for use in uncrewed aerial vehicles that need to detect, track, and recognize distant targets in dynamic environments is also discussed. Our avian eye-inspired perovskite artificial vision system marks a notable advance in bioinspired artificial visions.

Soft Bioelectronics Using Nanomaterials and Nanostructures for Neuroengineering.

The identification of neural networks for large areas and the regulation of neuronal activity at the single-neuron scale have garnered considerable attention in neuroscience. In addition, detecting biochemical molecules and electrically, optically, and chemically controlling neural functions are key research issues. However, conventional rigid and bulky bioelectronics face challenges for neural applications, including mechanical mismatch, unsatisfactory signal-to-noise ratio, and poor integration of multifunctional components, thereby degrading the sensing and modulation performance, long-term stability and biocompatibility, and diagnosis and therapy efficacy. Implantable bioelectronics have been developed to be mechanically compatible with the brain environment by adopting advanced geometric designs and utilizing intrinsically stretchable materials, but such advances have not been able to address all of the aforementioned challenges.Recently, the exploration of nanomaterial synthesis and nanoscale fabrication strategies has facilitated the design of unconventional soft bioelectronics with mechanical properties similar to those of neural tissues and submicrometer-scale resolution comparable to typical neuron sizes. The introduction of nanotechnology has provided bioelectronics with improved spatial resolution, selectivity, single neuron targeting, and even multifunctionality. As a result, this state-of-the-art nanotechnology has been integrated with bioelectronics in two main types, i.e., bioelectronics integrated with synthesized nanomaterials and bioelectronics with nanoscale structures. The functional nanomaterials can be synthesized and assembled to compose bioelectronics, allowing easy customization of their functionality to meet specific requirements. The unique nanoscale structures implemented with the bioelectronics could maximize the performance in terms of sensing and stimulation. Such soft nanobioelectronics have demonstrated their applicability for neuronal recording and modulation over a long period at the intracellular level and incorporation of multiple functions, such as electrical, optical, and chemical sensing and stimulation functions.In this Account, we will discuss the technical pathways in soft bioelectronics integrated with nanomaterials and implementing nanostructures for application to neuroengineering. We traced the historical development of bioelectronics from rigid and bulky structures to soft and deformable devices to conform to neuroengineering requirements. Recent approaches that introduced nanotechnology into neural devices enhanced the spatiotemporal resolution and endowed various device functions. These soft nanobioelectronic technologies are discussed in two categories: bioelectronics with synthesized nanomaterials and bioelectronics with nanoscale structures. We describe nanomaterial-integrated soft bioelectronics exhibiting various functionalities and modalities depending on the integrated nanomaterials. Meanwhile, soft bioelectronics with nanoscale structures are explained with their superior resolution and unique administration methods. We also exemplified the neural sensing and stimulation applications of soft nanobioelectronics across various modalities, showcasing their clinical applications in the treatment of neurological diseases, such as brain tumors, epilepsy, and Parkinson's disease. Finally, we discussed the challenges and direction of next-generation technologies.

Low-impedance tissue-device interface using homogeneously conductive hydrogels chemically bonded to stretchable bioelectronics.

Stretchable bioelectronics has notably contributed to the advancement of continuous health monitoring and point-of-care type health care. However, microscale nonconformal contact and locally dehydrated interface limit performance, especially in dynamic environments. Therefore, hydrogels can be a promising interfacial material for the stretchable bioelectronics due to their unique advantages including tissue-like softness, water-rich property, and biocompatibility. However, there are still practical challenges in terms of their electrical performance, material homogeneity, and monolithic integration with stretchable devices. Here, we report the synthesis of a homogeneously conductive polyacrylamide hydrogel with an exceptionally low impedance (~21 ohms) and a reasonably high conductivity (~24 S/cm) by incorporating polyaniline-decorated poly(3,4-ethylenedioxythiophene:polystyrene). We also establish robust adhesion (interfacial toughness: ~296.7 J/m2) and reliable integration between the conductive hydrogel and the stretchable device through on-device polymerization as well as covalent and hydrogen bonding. These strategies enable the fabrication of a stretchable multichannel sensor array for the high-quality on-skin impedance and pH measurements under in vitro and in vivo circumstances.

Phase-separated stretchable conductive nanocomposite to reduce contact resistance of skin electronics.

Skin electronics, facilitating a high-quality interface between external devices and human skin for recording physiological and/or electrophysiological signals as well as delivering external electrical and/or mechanical energy into the human body, has shown significant progress. However, achieving mechanically conformal contact and electrically low contact resistance at the device-skin interface remains challenging. Here, we propose a material strategy to potentially address such an issue by using phase separation of silver nanowires and silver nanoparticles (Ag NWs and Ag NPs) within a stretchable conductive nanocomposite (NC). This phase-separated NC ensures low contact resistance and high conductivity, which are key requirements in skin electronics, while maintaining excellent mechanical contact with the skin. To achieve phase separation, we hydrophobically treated the surfaces of Ag NWs and Ag NPs. Then, as the NC solidified, the solvent contained in the NC was slowly evaporated to sufficiently precipitate Ag NPs within the NC. As a result, the phase-separated NC exhibited high conductivity (~ 18,535 S cm-1), excellent stretchability (~ 80%), and low contact resistance on both the top and bottom NC surfaces (average ~ 0.132 Ω). The phase-separated NC has enabled implementation of high performance skin-mounted devices, including strain sensors, electrophysiological sensors, and a wearable heater.

Nanomaterial-Based Artificial Vision Systems: From Bioinspired Electronic Eyes to In-Sensor Processing Devices.

High-performance robotic vision empowers mobile and humanoid robots to detect and identify their surrounding objects efficiently, which enables them to cooperate with humans and assist human activities. For error-free execution of these robots' tasks, efficient imaging and data processing capabilities are essential, even under diverse and complex environments. However, conventional technologies fall short of meeting the high-standard requirements of robotic vision under such circumstances. Here, we discuss recent progress in artificial vision systems with high-performance imaging and data processing capabilities enabled by distinctive electrical, optical, and mechanical characteristics of nanomaterials surpassing the limitations of traditional silicon technologies. In particular, we focus on nanomaterial-based electronic eyes and in-sensor processing devices inspired by biological eyes and animal visual recognition systems, respectively. We provide perspectives on key nanomaterials, device components, and their functionalities, as well as explain the remaining challenges and future prospects of the artificial vision systems.

Flexible and Stretchable Light-Emitting Diodes and Photodetectors for Human-Centric Optoelectronics.

Optoelectronic devices with unconventional form factors, such as flexible and stretchable light-emitting or photoresponsive devices, are core elements for the next-generation human-centric optoelectronics. For instance, these deformable devices can be utilized as closely fitted wearable sensors to acquire precise biosignals that are subsequently uploaded to the cloud for immediate examination and diagnosis, and also can be used for vision systems for human-interactive robotics. Their inception was propelled by breakthroughs in novel optoelectronic material technologies and device blueprinting methodologies, endowing flexibility and mechanical resilience to conventional rigid optoelectronic devices. This paper reviews the advancements in such soft optoelectronic device technologies, honing in on various materials, manufacturing techniques, and device design strategies. We will first highlight the general approaches for flexible and stretchable device fabrication, including the appropriate material selection for the substrate, electrodes, and insulation layers. We will then focus on the materials for flexible and stretchable light-emitting diodes, their device integration strategies, and representative application examples. Next, we will move on to the materials for flexible and stretchable photodetectors, highlighting the state-of-the-art materials and device fabrication methods, followed by their representative application examples. At the end, a brief summary will be given, and the potential challenges for further development of functional devices will be discussed as a conclusion.

Soft Bioelectronics for Neuroengineering: New Horizons in the Treatment of Brain Tumor and Epilepsy.

Soft bioelectronic technologies for neuroengineering have shown remarkable progress, which include novel soft material technologies and device design strategies. Such technological advances that are initiated from fundamental brain science are applied to clinical neuroscience and provided meaningful promises for significant improvement in the diagnosis efficiency and therapeutic efficacy of various brain diseases recently. System-level integration strategies in consideration of specific disease circumstances can enhance treatment effects further. Here, recent advances in soft implantable bioelectronics for neuroengineering, focusing on materials and device designs optimized for the treatment of intracranial disease environments, are reviewed. Various types of soft bioelectronics for neuroengineering are categorized and exemplified first, and then details for the sensing and stimulating device components are explained. Next, application examples of soft implantable bioelectronics to clinical neuroscience, particularly focusing on the treatment of brain tumor and epilepsy are reviewed. Finally, an ideal system of soft intracranial bioelectronics such as closed-loop-type fully-integrated systems is presented, and the remaining challenges for their clinical translation are discussed.

Ultrathin Self-Powered Heavy-Metal-Free Cu-In-Se Quantum Dot Photodetectors for Wearable Health Monitoring.

Mechanically deformable photodetectors (PDs) are key device components for wearable health monitoring systems based on photoplethysmography (PPG). Achieving high detectivity, fast response time, and an ultrathin form factor in the PD is highly needed for next-generation wearable PPG systems. Self-powered operation without a bulky power-supply unit is also beneficial for point-of-care application. Here, we propose ultrathin self-powered PDs using heavy-metal-free Cu-In-Se quantum dots (QDs), which enable high-performance wearable PPG systems. Although the light-absorbing QD layer is extremely thin (∼40 nm), the developed PD exhibits excellent performance (specific detectivity: 2.10 × 1012 Jones, linear dynamic range: 102 dB, and spectral range: 250-1050 nm at zero bias), which is comparable to that of conventional rigid QD-PDs employing thick Pb-chalcogenide QD layers. This is attributed to material and device strategies─materials that include Cu-In-Se QDs, a MoS2-nanosheet-blended poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) hole transport layer, a ZnO nanoparticle electron transport layer, Ag and ITO electrodes, and an ultrathin form factor (∼120 nm except the electrodes) that enable excellent mechanical deformability. These allow the successful application of QD-PDs to a wearable system for real-time PPG monitoring, expanding their potential in the field of mobile bioelectronics.

Highly Efficient Nitrogen-Fixing Microbial Hydrogel Device for Sustainable Solar Hydrogen Production.

Conversion of sunlight and organic carbon substrates to sustainable energy sources through microbial metabolism has great potential for the renewable energy industry. Despite recent progress in microbial photosynthesis, the development of microbial platforms that warrant efficient and scalable fuel production remains in its infancy. Efficient transfer and retrieval of gaseous reactants and products to and from microbes are particular hurdles. Here, inspired by water lily leaves floating on water, a microbial device designed to operate at the air-water interface and facilitate concomitant supply of gaseous reactants, smooth capture of gaseous products, and efficient sunlight delivery is presented. The floatable device carrying Rhodopseudomonas parapalustris, of which nitrogen fixation activity is first determined through this study, exhibits a hydrogen production rate of 104 mmol h-1  m-2 , which is 53 times higher than that of a conventional device placed at a depth of 2 cm in the medium. Furthermore, a scaled-up device with an area of 144 cm2 generates hydrogen at a high rate of 1.52 L h-1  m-2 . Efficient nitrogen fixation and hydrogen generation, low fabrication cost, and mechanical durability corroborate the potential of the floatable microbial device toward practical and sustainable solar energy conversion.

Metal-Like Stretchable Nanocomposite Using Locally-Bundled Nanowires for Skin-Mountable Devices.

Stretchable conductive nanocomposites have been intensively studied for wearable bioelectronics. However, development of nanocomposites that simultaneously feature metal-like conductivity(> 100 000 S cm-1 ) and high stretchability (> 100%) for high-performance skin-mountable devices is still extremely challenging. Here a material strategy for such a nanocomposite is presented by using local bundling of silver nanowires stabilized with dual ligands (i.e., 1-propanethiols and 1-decanethiols). When the nanocomposite is solidified via solvent evaporation under a highly humid condition, the nanowires in the organic solution are bundled and stabilized. The resulting locally-bundled nanowires lower contact resistance while maintain their percolation network, leading to high conductivity. Dual ligands of 1-propanethiol and 1-decanethiol further boost up the conductivity. As a result, a nanocomposite with both high conductivity of ≈122,120 S cm-1 and high stretchability of ≈200% is obtained. Such superb electrical and mechanical properties are critical for various applications in skin-like electronics, and herein, a wearable thermo-stimulation device is demonstrated.

Minimally-Invasive and In-Vivo Hydrogel Patterning Method for In Situ Fabrication of Implantable Hydrogel Devices.

Despite advances in a wide range of device applications of hydrogels, including implantable ones, a method for deploying patterned hydrogel devices into the body in a minimally-invasive manner is not available yet. However, in situ patterning of the hydrogel in vivo has an obvious advantage, by which incision surgery for implantation of the hydrogel device can be avoided. Here, a minimally-invasive and in vivo hydrogel patterning method for in situ fabrication of implantable hydrogel devices is presented. The sequential application of injectable hydrogels and enzymes, with assistance of minimally-invasive surgical instruments, enables the in vivo and in situ hydrogel patterning. This patterning method can be achieved by adopting an appropriate combination of the sacrificial mold hydrogel and the frame hydrogel, in consideration of unique material properties of the hydrogels such as high softness, facile mass transfer, biocompatibility, and diverse crosslinking mechanisms. In vivo and in situ patterning of the hydrogels functionalized with nanomaterials is also demonstrated to fabricate the wireless heater and tissue scaffold, showcasing broad applicability of the patterning method.

Floatable photocatalytic hydrogel nanocomposites for large-scale solar hydrogen production.

Storing solar energy in chemical bonds aided by heterogeneous photocatalysis is desirable for sustainable energy conversion. Despite recent progress in designing highly active photocatalysts, inefficient solar energy and mass transfer, the instability of catalysts and reverse reactions impede their practical large-scale applications. Here we tackle these challenges by designing a floatable photocatalytic platform constructed from porous elastomer-hydrogel nanocomposites. The nanocomposites at the air-water interface feature efficient light delivery, facile supply of water and instantaneous gas separation. Consequently, a high hydrogen evolution rate of 163 mmol h-1 m-2 can be achieved using Pt/TiO2 cryoaerogel, even without forced convection. When fabricated in an area of 1 m2 and incorporated with economically feasible single-atom Cu/TiO2 photocatalysts, the nanocomposites produce 79.2 ml of hydrogen per day under natural sunlight. Furthermore, long-term stable hydrogen production in seawater and highly turbid water and photoreforming of polyethylene terephthalate demonstrate the potential of the nanocomposites as a commercially viable photocatalytic system.