Permeable Bioelectronics toward Biointegrated Systems.

Bioelectronics integrates electronics with biological organs, sustaining the natural functions of the organs. Organs dynamically interact with the external environment, managing internal equilibrium and responding to external stimuli. These interactions are crucial for maintaining homeostasis. Additionally, biological organs possess a soft and stretchable nature; encountering objects with differing properties can disrupt their function. Therefore, when electronic devices come into contact with biological objects, the permeability of these devices, enabling interactions and substance exchanges with the external environment, and the mechanical compliance are crucial for maintaining the inherent functionality of biological organs. This review discusses recent advancements in soft and permeable bioelectronics, emphasizing materials, structures, and a wide range of applications. The review also addresses current challenges and potential solutions, providing insights into the integration of electronics with biological organs.

Janus Membrane-Based Wearable pH Sensor with Sweat Absorption, Gas Permeability, and Self-Adhesiveness.

Wearable biomedical sensors have enabled noninvasive and continuous physiological monitoring for daily health management and early detection of chronic diseases. Among biomedical sensors, wearable pH sensors attracted significant interest, as pH influences most biological reactions. However, conformable pH sensors that have sweat absorption ability, are self-adhesive to the skin, and are gas permeable remain largely unexplored. In this study, we present a pioneering approach to this problem by developing a Janus membrane-based pH sensor with self-adhesiveness on the skin. The sensor is composed of a hydrophobic polyurethane-polydimethylsiloxane porous hundreds nanometer-thick substrate and a hydrophilic poly(vinyl alcohol)-poly(acrylic acid) porous nanofiber layer. This Janus membrane exhibits a thickness of around 10 µm, providing a conformable adhesion to the skin. The simultaneous realization of solution absorption, gas permeability, and self-adhesiveness makes it suitable for long-term continuous monitoring without compromising the comfort of the wearer. The pH sensor was tested successfully for continuous monitoring for 7.5 h, demonstrating its potential for stable analysis of skin health conditions. The Janus membrane-based pH sensor holds significant promise for comprehensive skin health monitoring and wearable biomedical applications.

All-solution-processed ultraflexible wearable sensor enabled with universal trilayer structure for organic optoelectronic devices.

All-solution-processed organic optoelectronic devices can enable the large-scale manufacture of ultrathin wearable electronics with integrated diverse functions. However, the complex multilayer-stacking device structure of organic optoelectronics poses challenges for scalable production. Here, we establish all-solution processes to fabricate a wearable, self-powered photoplethysmogram (PPG) sensor. We achieve comparable performance and improved stability compared to complex reference devices with evaporated electrodes by using a trilayer device structure applicable to organic photovoltaics, photodetectors, and light-emitting diodes. The PPG sensor array based on all-solution-processed organic light-emitting diodes and photodetectors can be fabricated on a large-area ultrathin substrate to achieve long storage stability. We integrate it with a large-area, all-solution-processed organic solar module to realize a self-powered health monitoring system. We fabricate high-throughput wearable electronic devices with complex functions on large-area ultrathin substrates based on organic optoelectronics. Our findings can advance the high-throughput manufacture of ultrathin electronic devices integrating complex functions.

Functional soft robotic composites based on organic photovoltaic and dielectric elastomer actuator.

Improving the energy efficiency of robots remains a crucial challenge in soft robotics, with energy harvesting emerging as a promising approach to address it. This study presents a functional soft robotic composite called OPV-DEA, which integrates flexible organic photovoltaic (OPV) and dielectric elastomer actuator (DEA). The composite can simultaneously generate electrostatic bending actuation and harvest energy from external lights. Owing to its simplicity and inherent flexibility, the OPV-DEA is poised to function as a fundamental building block for soft robots. This study aimed to validate this concept by initially establishing the fabrication process of OPV-DEA. Subsequently, experimental samples are fabricated and characterized. The results show that the samples exhibit a voltage-controllable bending actuation of up to 15.6° and harvested power output of 1.35 mW under an incident power irradiance of 11.7 mW/cm2. These performances remain consistent even after 1000 actuation cycles. Finally, to demonstrate the feasibility of soft robotic applications, an untethered swimming robot equipped with two OPV-DEAs is fabricated and tested. The robot demonstrates swimming at a speed of 21.7 mm/s. The power consumption of the robot is dominated by a high-voltage DC-DC converter, with a value approximately 1.5 W. As a result, the on-board OPVs cannot supply the necessary energy during locomotion simultaneously. Instead, they contribute to the overall system by charging a battery used for the controller on board. Nevertheless, these findings suggest that the OPV-DEA could pave the way for the development of an unprecedented range of functional soft robots.

Waterproof and ultraflexible organic photovoltaics with improved interface adhesion.

Ultraflexible organic photovoltaics have emerged as a potential power source for wearable electronics owing to their stretchability and lightweight nature. However, waterproofing ultraflexible organic photovoltaics without compromising mechanical flexibility and conformability remains challenging. Here, we demonstrate waterproof and ultraflexible organic photovoltaics through the in-situ growth of a hole-transporting layer to strengthen interface adhesion between the active layer and anode. Specifically, a silver electrode is deposited directly on top of the active layers, followed by thermal annealing treatment. Compared with conventional sequentially-deposited hole-transporting layers, the in-situ grown hole-transporting layer exhibits higher thermodynamic adhesion between the active layers, resulting in better waterproofness. The fabricated 3 µm-thick organic photovoltaics retain 89% and 96% of their pristine performance after immersion in water for 4 h and 300 stretching/releasing cycles at 30% strain under water, respectively. Moreover, the ultraflexible devices withstand a machine-washing test with such a thin encapsulation layer, which has never been reported. Finally, we demonstrate the universality of the strategy for achieving waterproof solar cells.

Flexible Solution-Processed Electron-Transport-Layer-Free Organic Photovoltaics for Indoor Application.

Organic photovoltaics (OPVs) have unique advantages of low weight, mechanical flexibility, and solution processability, which make them exceptionally suitable for integrating low-power Internet of Things devices. However, achieving improved operational stability together with solution processes that are applicable to large-scale fabrication remains challenging. Their major limitation arises due to the instable factors that occur both inside the thick active film and from the ambient environment, which cannot be completely resolved via the current encapsulation techniques used for flexible OPVs. Additionally, thin active layers are highly vulnerable to point defects, which result in low yield rates and impede the laboratory-to-industry translation. In this study, flexible fully solution-processed OPVs with improved indoor efficiency and long-term operational stability than that of conventional OPVs with evaporated electrodes are achieved. Benefiting from the oxygen and water vapor permeation barrier of the spontaneously formed gallium oxide layers on the exposed eutectic gallium-indium surface, fast degradation of the OPVs with thick active layers is prevented, maintaining 93% of its initial Pmax after 5000 min of indoor operation under 1000 lx light-emitting diode (LED) illumination. Additionally, by using the thick active layer, spin-coated silver nanowires could be directly used as bottom electrodes without complicated flattening processes, thereby substantially simplifying the fabrication process and proposing a promising manufacturing technique for devices with high-throughput energy demands.

Surface-Energy-Mediated Interfacial Adhesion for Mechanically Robust Ultraflexible Organic Photovoltaics.

Insufficient interfacial adhesion is a widespread problem across multilayered devices that undermines their reliability. In flexible organic photovoltaics (OPVs), poor interfacial adhesion can accelerate degradation and failure under mechanical deformations due to the intrinsic brittleness and mismatching mechanical properties between functional layers. We introduce an argon plasma treatment for OPV devices, which yields 58% strengthening in interfacial adhesion between an active layer and a MoOX hole transport layer, thus contributing to mechanical reliability. The improved adhesion is attributed to the increased surface energy of the active layer that occurred after the mild argon plasma treatment. The mechanically stabilized interface retards the flexible device degradation induced by mechanical stress and maintains a power conversion efficiency of 94.8% after 10,000 cycles of bending with a radius of 2.5 mm. In addition, a fabricated 3 µm thick ultraflexible OPV device shows excellent mechanical robustness, retaining 91.0% of the initial efficiency after 1000 compressing-stretching cycles with a 40% compression ratio. The developed ultraflexible OPV devices can operate stably at the maximum power point under continuous 1 sun illumination for 500 min with an 89.3% efficiency retention. Overall, we validate a simple interfacial linking strategy for efficient and mechanically robust flexible and ultraflexible OPVs.

Simple Method for Creating Hydrophobic Ultraflexible Photovoltaics.

Optoelectronic devices, such as photodetectors and photovoltaics, are susceptible to surface contamination or water damage that can lead to reductions in performance or stability. Applying superhydrophobic coatings to these devices can introduce self-cleaning behavior and water resistance to extend their lifetime and improve their efficiency. However, existing methods for inducing superhydrophobicity have not been compatible with ultraflexible devices because of their thickness and complexity requirements. In this work, we introduce a procedure for inducing superhydrophobic and self-cleaning behavior on ultraflexible components using a combination of shrinkage-induced wrinkles and a low-surface-energy coating. We apply these techniques to an ultraflexible organic photovoltaics and demonstrate excellent hydrophobicity and self-cleaning behavior.

Ultrathin Hydrogel Films toward Breathable Skin-Integrated Electronics.

On-skin electronics that offer revolutionary capabilities in personalized diagnosis, therapeutics, and human-machine interfaces require seamless integration between the skin and electronics. A common question remains whether an ideal interface can be introduced to directly bridge thin-film electronics with the soft skin, allowing the skin to breathe freely and the skin-integrated electronics to function stably. Here, an ever-thinnest hydrogel is reported that is compliant to the glyphic lines and subtle minutiae on the skin without forming air gaps, produced by a facile cold-lamination method. The hydrogels exhibit high water-vapor permeability, allowing nearly unimpeded transepidermal water loss and free breathing of the skin underneath. Hydrogel-interfaced flexible (opto)electronics without causing skin irritation or accelerated device performance deterioration are demonstrated. The long-term applicability is recorded for over one week. With combined features of extreme mechanical compliance, high permeability, and biocompatibility, the ultrathin hydrogel interface promotes the general applicability of skin-integrated electronics.

Antimicrobial second skin using copper nanomesh.

The functional support and advancement of our body while preserving inherent naturalness is one of the ultimate goals of bioengineering. Skin protection against infectious pathogens is an application that requires common and long-term wear without discomfort or distortion of the skin functions. However, no antimicrobial method has been introduced to prevent cross-infection while preserving intrinsic skin conditions. Here, we propose an antimicrobial skin protection platform copper nanomesh, which prevents cross-infectionmorphology, temperature change rate, and skin humidity. Copper nanomesh exhibited an inactivation rate of 99.99% for Escherichia coli bacteria and influenza virus A within 1 and 10 min, respectively. The thin and porous nanomesh allows for conformal coating on the fingertips, without significant interference with the rate of skin temperature change and humidity. Efficient cross-infection prevention and thermal transfer of copper nanomesh were demonstrated using direct on-hand experiments.

Solution-Processed Electron-Transport Layer-free Organic Photovoltaics with Liquid Metal Cathodes.

Flexible, lightweight, and large-area solar cells provide new power supply opportunities in the renewable energy field and facilitate the supply of power to internet-of-things devices and wearable devices. The choice of printing process technologies is a key parameter for such flexible power sources because of their energy-saving process technology and high throughput rate. In addition to selecting the appropriate printing method for the active and charge transport layers, the development of printed electrodes is critical. Numerous printable materials have been developed to replace conventional evaporated top electrodes. However, achieving fully solution-processed organic photovoltaics (OPVs) with power conversion efficiency (PCE) comparable to OPVs with vacuum-deposited transparent and top electrodes is challenging. This is because of the difficulty of forming a uniform interface between the top solution-processed electrode and the active layers while preventing deterioration. In this study, an electron transport layer-free, eutectic gallium-indium (EGaIn) top-cathode strategy was developed and a record PCE of 12.7% in fully solution-processed, flexible OPVs was achieved. Direct coating of EGaIn on the active layer, in a nitrogen atmosphere, is conducive for energy band matching and obtaining physically perfect interfaces without any penetrations or voids. An average PCE of 14.1% and enhanced operating stability, comparable to conventional OPVs, were achieved with indium tin oxide transparent electrodes by eliminating the electron-transport layer. The fully solution-processed flexible OPVs fabricated with the embedded silver nanowire strategy in ultrathin transparent polyimide, achieved an average PCE of 12.7%, representing a promising technique to meet green and high-throughput energy demands.

Ultrathin and Efficient Organic Photovoltaics with Enhanced Air Stability by Suppression of Zinc Element Diffusion.

Ultrathin (thickness less than 10 µm) organic photovoltaics (OPVs) can be applied to power soft robotics and wearable electronics. In addition to high power conversion efficiency, stability under various environmental stresses is crucial for the application of ultrathin OPVs. In this study, the authors realize highly air-stable and ultrathin (≈3 µm) OPVs that possess high efficiency (15.8%) and an outstanding power-per-weight ratio of 33.8 W g-1 . Dynamic secondary-ion mass spectrometry is used to identify Zn diffusion from the electron transport layer zinc oxide (ZnO) to the interface of photoactive layer; this diffusion results in the degradation of the ultrathin OPVs in air. The suppression of the Zn diffusion by a chelating strategy results in stable ultrathin OPVs that maintain 89.6% of their initial efficiency after storage for 1574 h in air at room temperature under dark conditions and 92.4% of their initial efficiency after annealing for 172 h at 85 °C in air under dark conditions. The lightweight and stable OPVs also possess excellent deformability with 87.3% retention of the initial performance after 5000 cycles of a compressing-stretching test with 33% compression.

Smart Face Mask Based on an Ultrathin Pressure Sensor for Wireless Monitoring of Breath Conditions.

A smart face mask that can conveniently monitor breath information is beneficial for maintaining personal health and preventing the spread of diseases. However, some challenges still need to be addressed before such devices can be of practical use. One key challenge is to develop a pressure sensor that is easily triggered by low pressure and has excellent stability as well as electrical and mechanical properties. In this study, a wireless smart face mask is designed by integrating an ultrathin self-powered pressure sensor and a compact readout circuit with a normal face mask. The pressure sensor is the thinnest (totally compressed thickness of ≈5.5 µm) and lightest (total weight of ≈4.5 mg) electrostatic pressure sensor capable of achieving a peak open-circuit voltage of up to ≈10 V when stimulated by airflow, which endows the sensor with the advantage of readout circuit miniaturization and makes the breath-monitoring system portable and wearable. To demonstrate the capabilities of the smart face mask, it is used to wirelessly measure and analyze the various breath conditions of multiple testers.

Developing the Nondevelopable: Creating Curved-Surface Electronics from Nonstretchable Devices.

The incorporation of electronics onto curved surfaces promises to bring new levels of intelligence to the ergonomic, aesthetic, aerodynamic, and optical surfaces that are ever-present in our lives. However, since many of these surfaces have 2D (i.e., nondevelopable) curvature, they cannot be formed from the deformation of a flat, nonstretchable sheet. This means that curved electronics cannot capitalize on the rapid technological advances taking place in the field of ultrathin electronics, since ultrathin devices, though ultraflexible, are not stretchable. In this work, a shrink-based paradigm is presented to apply such thin-film electronics to nondevelopable surfaces, expanding the capabilities of current nondevelopable electronics, and linking future developments in thin-film technology to similar developments in curved devices. The wrinkling of parylene-based devices and the effects of shrinkage on common electrical components are examined, culminating in shrinkable touch sensors and organic photovoltaics, laminated to various nondevelopable surfaces without loss of performance.

Direct gold bonding for flexible integrated electronics.

Flexible and stable interconnections are critical for the next generation of shape-conformable and wearable electronics. These interconnections should have metal-like conductivity and sufficiently low stiffness that does not compromise the flexibility of the device; moreover, they must be achieved using low-temperature processes to prevent device damage. However, conventional interconnection bonding methods require additional adhesive layers, making it challenging to achieve these characteristics simultaneously. Here, we develop and characterize water vapor plasma­assisted bonding (WVPAB) that enables direct bonding of gold electrodes deposited on ultrathin polymer films. WVPAB bonds rough gold electrodes at room temperature and atmospheric pressure in ambient air. Hydroxyl groups generated by the plasma assist bonding between two gold surfaces, allowing the formation of a strong and stable interface. The applicability of WVPAB-mediated connections to ultrathin electronic systems was also demonstrated, and ultraflexible organic photovoltaics and light-emitting diodes fabricated on separate films were successfully interconnected via ultrathin wiring films.

Well-rounded devices: the fabrication of electronics on curved surfaces - a review.

With the arrival of the internet of things and the rise of wearable computing, electronics are playing an increasingly important role in our everyday lives. Until recently, however, the rigid angular nature of traditional electronics has prevented them from being integrated into many of the organic, curved shapes that interface with our bodies (such as ergonomic equipment or medical devices) or the natural world (such as aerodynamic or optical components). In the past few years, many groups working in advanced manufacturing and soft robotics have endeavored to develop strategies for fabricating electronics on these curved surfaces. This is their story. In this work, we describe the motivations, challenges, methodologies, and applications of curved electronics, and provide a outlook for this promising field.

Simultaneous measurement of contractile force and field potential of dynamically beating human iPS cell-derived cardiac cell sheet-tissue with flexible electronics.

Human induced pluripotent stem (iPS) cell-derived cardiomyocytes are used for in vitro pharmacological and pathological studies worldwide. In particular, the functional assessment of cardiac tissues created from iPS cell-derived cardiomyocytes is expected to provide precise prediction of drug effects and thus streamline the process of drug development. However, the current format of electrophysiological and contractile assessment of cardiomyocytes on a rigid substrate is not appropriate for cardiac tissues that beat dynamically. Here, we show a novel simultaneous measurement system for contractile force and extracellular field potential of iPS cell-derived cardiac cell sheet-tissues using 500 nm-thick flexible electronic sheets. It was confirmed that the developed system is applicable for pharmacological studies and assessments of excitation-contraction coupling-related parameters, such as the electro-mechanical window. Our results indicate that flexible electronics with cardiac tissue engineering provide an advanced platform for drug development. This system will contribute to gaining new insight in pharmacological study of human cardiac function.

Self-powered ultraflexible photonic skin for continuous bio-signal detection via air-operation-stable polymer light-emitting diodes.

Ultraflexible optical devices have been used extensively in next-generation wearable electronics owing to their excellent conformability to human skins. Long-term health monitoring also requires the integration of ultraflexible optical devices with an energy-harvesting power source; to make devices self-powered. However, system-level integration of ultraflexible optical sensors with power sources is challenging because of insufficient air operational stability of ultraflexible polymer light-emitting diodes. Here we develop an ultraflexible self-powered organic optical system for photoplethysmogram monitoring by combining air-operation-stable polymer light-emitting diodes, organic solar cells, and organic photodetectors. Adopting an inverted structure and a doped polyethylenimine ethoxylated layer, ultraflexible polymer light-emitting diodes retain 70% of the initial luminance even after 11.3 h of operation under air. Also, integrated optical sensors exhibit a high linearity with the light intensity exponent of 0.98 by polymer light-emitting diode. Such self-powered, ultraflexible photoplethysmogram sensors perform monitoring of blood pulse signals as 77 beats per minute.

Recent Progress of Flexible Image Sensors for Biomedical Applications.

Flexible image sensors have attracted increasing attention as new imaging devices owing to their lightness, softness, and bendability. Since light can measure inside information from outside of the body, optical-imaging-based approaches, such as X-rays, are widely used for disease diagnosis in hospitals. Unlike conventional sensors, flexible image sensors are soft and can be directly attached to a curved surface, such as the skin, for continuous measurement of biometric information with high accuracy. Therefore, they are expected to gain wide application to wearable devices, as well as home medical care. Herein, the application of such sensors to the biomedical field is introduced. First, their individual components, photosensors, and switching elements, are explained. Then, the basic parameters used to evaluate the performance of each of these elements and the image sensors are described. Finally, examples of measuring the dynamic and static biometric information using flexible image sensors, together with relevant real-world measurement cases, are presented. Furthermore, recent applications of the flexible image sensors in the biomedical field are introduced.

Robust metal ion-chelated polymer interfacial layer for ultraflexible non-fullerene organic solar cells.

Achieving high power conversion efficiency and good mechanical robustness is still challenging for the ultraflexible organic solar cells. Interlayers simultaneously having good mechanical robustness and good chemical compatibility with the active layer are highly desirable. In this work, we present an interlayer of Zn2+-chelated polyethylenimine (denoted as PEI-Zn), which can endure a maximum bending strain over twice as high as that of ZnO and is chemically compatible with the recently emerging efficient nonfullerene active layers. On 1.3 µm polyethylene naphthalate substrates, ultraflexible nonfullerene solar cells with the PEI-Zn interlayer display a power conversion efficiency of 12.3% on PEDOT:PSS electrodes and 15.0% on AgNWs electrodes. Furthermore, the ultraflexible cells show nearly unchanged power conversion efficiency during 100 continuous compression-flat deformation cycles with a compression ratio of 45%. At the end, the ultraflexible cell is demonstrated to be attached onto the finger joint and displays reversible current output during the finger bending-spreading.