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.

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.

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.

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.

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.

Soft Bioelectronics Based on Nanomaterials.

Recent advances in nanostructured materials and unconventional device designs have transformed the bioelectronics from a rigid and bulky form into a soft and ultrathin form and brought enormous advantages to the bioelectronics. For example, mechanical deformability of the soft bioelectronics and thus its conformal contact onto soft curved organs such as brain, heart, and skin have allowed researchers to measure high-quality biosignals, deliver real-time feedback treatments, and lower long-term side-effects in vivo. Here, we review various materials, fabrication methods, and device strategies for flexible and stretchable electronics, especially focusing on soft biointegrated electronics using nanomaterials and their composites. First, we summarize top-down material processing and bottom-up synthesis methods of various nanomaterials. Next, we discuss state-of-the-art technologies for intrinsically stretchable nanocomposites composed of nanostructured materials incorporated in elastomers or hydrogels. We also briefly discuss unconventional device design strategies for soft bioelectronics. Then individual device components for soft bioelectronics, such as biosensing, data storage, display, therapeutic stimulation, and power supply devices, are introduced. Afterward, representative application examples of the soft bioelectronics are described. A brief summary with a discussion on remaining challenges concludes the review.

Electric-Field-Mediated In-Sensor Alignment of Antibody's Orientation to Enhance the Antibody-Antigen Binding for Ultrahigh Sensitivity Sensors.

Applying an electric-field (E-field) during antibody immobilization aligns the orientation of the antibody on the biosensor surface, thereby enhancing the binding probability between the antibody and antigen and maximizing the sensitivity of the biosensor. In this study, a biosensor with enhanced antibody-antigen binding probability was developed using the alignment of polar antibodies (immunoglobulin G [IgG]) under an E-field applied inside the interdigitated electrodes. The optimal alignment condition was first theoretically calculated and then experimentally confirmed by comparing the impedance change before and after the alignment of IgG (a purified anti-ß-amyloid antibody). With the optimized condition, the impedance change of the biosensor was maximized because of the alignment of IgG orientation on the sensor surface; the detection sensitivity of the antigen amyloid-beta 1-42 was also maximized. The E-field-based in-sensor alignment of antibodies is an easy and effective method for enhancing biosensor sensitivity.

Toward Full-Color Electroluminescent Quantum Dot Displays.

Colloidal quantum dots (QDs) exhibit unique characteristics such as facile color tunability, pure color emission with extremely narrow bandwidths, high luminescence efficiency, and high photostability. In addition, quantum dot light-emitting diodes (QLEDs) feature bright electroluminescence, low turn-on voltage, and ultrathin form factor, making them a promising candidate for next-generation displays. To achieve the overarching goal of the full-color display based on the electroluminescence of QDs, however it is essential to enhance the performance of QLEDs further for each color (e.g., red, green, and blue; RGB) and develop novel techniques for patterning RGB QD pixels without cross-contamination. Here, we present state-of-the-art material, process, and device technologies for full-color QLED-based displays. First, we highlight recent advances in the development of efficient red-, green-, and blue-monochromatic QLEDs. In particular, we focus on the progress of heavy-metal-free QLEDs. Then, we describe patterning techniques for individual RGB QDs to fabricate pixelated displays. Finally, we briefly summarize applications of such QLEDs, presenting the possibility of full-color QLED-based displays.

Wafer-Scale Production of Transition Metal Dichalcogenides and Alloy Monolayers by Nanocrystal Conversion for Large-Scale Ultrathin Flexible Electronics.

Two-dimensional (2D) transition metal dichalcogenide (TMD) layers are unit-cell thick materials with tunable physical properties according to their size, morphology, and chemical composition. Their transition of lab-scale research to industrial-scale applications requires process development for the wafer-scale growth and scalable device fabrication. Herein, we report on a new type of atmospheric pressure chemical vapor deposition (APCVD) process that utilizes colloidal nanoparticles as process-scalable precursors for the wafer-scale production of TMD monolayers. Facile uniform distribution of nanoparticle precursors on the entire substrate leads to the wafer-scale uniform synthesis of TMD monolayers with the controlled size and morphology. Composition-controlled TMD alloy monolayers with tunable bandgaps can be produced by simply mixing dual nanoparticle precursor solutions in the desired ratio. We also demonstrate the fabrication of ultrathin field-effect transistors and flexible electronics with uniformly controlled performance by using TMD monolayers.

Material Design and Fabrication Strategies for Stretchable Metallic Nanocomposites.

Stretchable conductive nanocomposites fabricated by integrating metallic nanomaterials with elastomers have become a vital component of human-friendly electronics, such as wearable and implantable devices, due to their unconventional electrical and mechanical characteristics. Understanding the detailed material design and fabrication strategies to improve the conductivity and stretchability of the nanocomposites is therefore important. This Review discusses the recent technological advances toward high performance stretchable metallic nanocomposites. First, the effect of the filler material design on the conductivity is briefly discussed, followed by various nanocomposite fabrication techniques to achieve high conductivity. Methods for maintaining the initial conductivity over a long period of time are also summarized. Then, strategies on controlled percolation of nanomaterials are highlighted, followed by a discussion regarding the effects of the morphology of the nanocomposite and postfabricated 3D structures on achieving high stretchability. Finally, representative examples of applications of such nanocomposites in biointegrated electronics are provided. A brief outlook concludes this Review.

Wearable and Implantable Soft Bioelectronics Using Two-Dimensional Materials.

Soft bioelectronics intended for application to wearable and implantable biomedical devices have attracted great attention from material scientists, device engineers, and clinicians because of their extremely soft mechanical properties that match with a variety of human organs and tissues, including the brain, heart, skin, eye, muscles, and neurons, as well as their wide diversity in device designs and biomedical functions that can be finely tuned for each specific case of applications. These unique features of the soft bioelectronics have allowed minimal mechanical and biological damage to organs and tissues integrated with bioelectronic devices and reduced side effects including inflammation, skin irritation, and immune responses even after long-term biointegration. These favorable properties for biointegration have enabled long-term monitoring of key biomedical indicators with high signal-to-noise ratio, reliable diagnosis of the patient's health status, and in situ feedback therapy with high treatment efficacy optimized for the requirements of each specific disease model. These advantageous device functions and performances could be maximized by adopting novel high-quality soft nanomaterials, particularly ultrathin two-dimensional (2D) materials, for soft bioelectronics. Two-dimensional materials are emerging material candidates for the channels and electrodes in electronic devices (semiconductors and conductors, respectively). They can also be applied to various biosensors and therapeutic actuators in soft bioelectronics. The ultrathin vertically layered nanostructure, whose layer number can be controlled in the synthesis step, and the horizontally continuous planar molecular structure, which can be found over a large area, have conferred unique mechanical, electrical, and optical properties upon the 2D materials. The atomically thin nanostructure allows mechanical softness and flexibility and high optical transparency of the device, while the large-area continuous thin film structure allows efficient carrier transport within the 2D plane. In addition, the quantum confinement effect in the atomically thin 2D layers introduces interesting optoelectronic properties and superb photodetecting capabilities. When fabricated as soft bioelectronic devices, these interesting and useful material features of the 2D materials enable unconventional device functions in biological and optical sensing, as well as superb performance in electrical and biochemical therapeutic actuations. In this Account, we first summarize the distinctive characteristics of the 2D materials in terms of the mechanical, optical, chemical, electrical, and biomedical aspects and then present application examples of the 2D materials to soft bioelectronic devices based on each aforementioned unique material properties. Among various kinds of 2D materials, we particularly focus on graphene and MoS2. The advantageous material features of graphene and MoS2 include ultrathin thickness, facile functionalization, large surface-to-volume ratio, biocompatibility, superior photoabsorption, and high transparency, which allow the development of high-performance multifunctional soft bioelectronics, such as a wearable glucose patch, a highly sensitive humidity sensor, an ultrathin tactile sensor, a soft neural probe, a soft retinal prosthesis, a smart endoscope, and a cell culture platform. A brief comparison of their characteristics and performances is also provided. Finally, this Account concludes with a future outlook on next-generation soft bioelectronics based on 2D materials.

High-performance stretchable conductive nanocomposites: materials, processes, and device applications.

Highly conductive and intrinsically stretchable electrodes are vital components of soft electronics such as stretchable transistors and circuits, sensors and actuators, light-emitting diode arrays, and energy harvesting devices. Many kinds of conducting nanomaterials with outstanding electrical and mechanical properties have been integrated with elastomers to produce stretchable conductive nanocomposites. Understanding the characteristics of these nanocomposites and assessing the feasibility of their fabrication are therefore critical for the development of high-performance stretchable conductors and electronic devices. We herein summarise the recent advances in stretchable conductors based on the percolation networks of nanoscale conductive fillers in elastomeric media. After discussing the material-, dimension-, and size-dependent properties of conductive fillers and their implications, we highlight various techniques that are used to reduce the contact resistance between the conductive filler materials. Furthermore, we categorize elastomer matrices with different stretchabilities and mechanical properties based on their polymeric chain structures. Then, we discuss the fabrication techniques of stretchable conductive nanocomposites toward their use in soft electronics. Finally, we provide representative examples of stretchable device applications and conclude the review with a brief outlook for future research.

Soft High-Resolution Neural Interfacing Probes: Materials and Design Approaches.

Neural interfacing probes are located between the nervous system and the implanted electronic device in order to acquire information on the complex neuronal activity and to reconstruct impaired neural connectivity. Despite remarkable advancement in recent years, conventional neural interfacing is still unable to completely accomplish these goals, especially in long-term brain interfacing. The major limitation arises from physical and mechanical differences between neural interfacing probes and neural tissues that cause local immune responses and production of scar cells near the interface. Therefore, neural interfaces should ideally be extremely soft and have the physical scale of cells to mitigate the boundary between biotic and abiotic systems. Soft materials for neural interfaces have been intensively investigated to improve both interfacing and long-term signal transmission. The design and fabrication of micro and nanoscale devices have drastically decreased the stiffness of probes and enabled single-neuron measurement. In this Mini Review, we discuss materials and design approaches for developing soft high-resolution neural probes intended for long-term brain interfacing and outline existent challenges for achieving next-generation neural interfacing probes.

Solution-processed thin films of semiconducting carbon nanotubes and their application to soft electronics.

Semiconducting single-walled carbon nanotube (SWNT) networks are promising for use as channel materials in field-effect transistors (FETs) in next-generation soft electronics, owing to their high intrinsic carrier mobility, mechanical flexibility, potential for low-cost production, and good processability. In this article, we review the recent progress related to carbon nanotube (CNT) devices in soft electronics by describing the materials and devices, processing methods, and example applications in soft electronic systems. First, solution-processed semiconducting SWNT deposition methods along with doping techniques used to achieve stable complementary metal-oxide-semiconductor devices are discussed. Various strategies for developing high-performance SWNT-based FETs, such as the proper material choices for the gates, dielectrics, and sources/drains of FETs, and methods of improving FET performance, such as hysteresis repression in SWNT-based FETs, are described next. These SWNT-based FETs have been used in flexible, stretchable, and wearable electronic devices to realize functionalities that could not be achieved using conventional silicon-based devices. We conclude this review by discussing the challenges faced by and outlook for CNT-based soft electronics.

Electronic sensor and actuator webs for large-area complex geometry cardiac mapping and therapy.

Curved surfaces, complex geometries, and time-dynamic deformations of the heart create challenges in establishing intimate, nonconstraining interfaces between cardiac structures and medical devices or surgical tools, particularly over large areas. We constructed large area designs for diagnostic and therapeutic stretchable sensor and actuator webs that conformally wrap the epicardium, establishing robust contact without sutures, mechanical fixtures, tapes, or surgical adhesives. These multifunctional web devices exploit open, mesh layouts and mount on thin, bio-resorbable sheets of silk to facilitate handling in a way that yields, after dissolution, exceptionally low mechanical moduli and thicknesses. In vivo studies in rabbit and pig animal models demonstrate the effectiveness of these device webs for measuring and spatially mapping temperature, electrophysiological signals, strain, and physical contact in sheet and balloon-based systems that also have the potential to deliver energy to perform localized tissue ablation.

A high-density, high-channel count, multiplexed µECoG array for auditory-cortex recordings.

Our understanding of the large-scale population dynamics of neural activity is limited, in part, by our inability to record simultaneously from large regions of the cortex. Here, we validated the use of a large-scale active microelectrode array that simultaneously records 196 multiplexed micro-electrocortigraphical (µECoG) signals from the cortical surface at a very high density (1,600 electrodes/cm(2)). We compared µECoG measurements in auditory cortex using a custom "active" electrode array to those recorded using a conventional "passive" µECoG array. Both of these array responses were also compared with data recorded via intrinsic optical imaging, which is a standard methodology for recording sound-evoked cortical activity. Custom active µECoG arrays generated more veridical representations of the tonotopic organization of the auditory cortex than current commercially available passive µECoG arrays. Furthermore, the cortical representation could be measured efficiently with the active arrays, requiring as little as 13.5 s of neural data acquisition. Next, we generated spectrotemporal receptive fields from the recorded neural activity on the active µECoG array and identified functional organizational principles comparable to those observed using intrinsic metabolic imaging and single-neuron recordings. This new electrode array technology has the potential for large-scale, temporally precise monitoring and mapping of the cortex, without the use of invasive penetrating electrodes.