E-Tattoos: Toward Functional but Imperceptible Interfacing with Human Skin.

The human body continuously emits physiological and psychological information from head to toe. Wearable electronics capable of noninvasively and accurately digitizing this information without compromising user comfort or mobility have the potential to revolutionize telemedicine, mobile health, and both human-machine or human-metaverse interactions. However, state-of-the-art wearable electronics face limitations regarding wearability and functionality due to the mechanical incompatibility between conventional rigid, planar electronics and soft, curvy human skin surfaces. E-Tattoos, a unique type of wearable electronics, are defined by their ultrathin and skin-soft characteristics, which enable noninvasive and comfortable lamination on human skin surfaces without causing obstruction or even mechanical perception. This review article offers an exhaustive exploration of e-tattoos, accounting for their materials, structures, manufacturing processes, properties, functionalities, applications, and remaining challenges. We begin by summarizing the properties of human skin and their effects on signal transmission across the e-tattoo-skin interface. Following this is a discussion of the materials, structural designs, manufacturing, and skin attachment processes of e-tattoos. We classify e-tattoo functionalities into electrical, mechanical, optical, thermal, and chemical sensing, as well as wound healing and other treatments. After discussing energy harvesting and storage capabilities, we outline strategies for the system integration of wireless e-tattoos. In the end, we offer personal perspectives on the remaining challenges and future opportunities in the field.

Free-Standing Carbon Nanotube Embroidered Graphene Film Electrode Array for Stable Neural Interfacing.

Implantable neural probes that are mechanically flexible yet robust are attractive candidates for achieving stable neural interfacing in the brain. Current flexible neural probes consist mainly of metal thin-film electrodes integrated on micrometer-thick polymer substrates, making it challenging to achieve electrode-tissue interfacing on the cellular scale. Here, we describe implantable neural probes that consist of robust carbon nanotube network embroidered graphene (CeG) films as free-standing recording microelectrodes. Our CeG film microelectrode arrays (CeG_MEAs) are ultraflexible yet mechanically robust, thus enabling cellular-scale electrode-tissue interfacing. Chronically implanted CeG_MEAs can stably track the activities of the same population of neurons over two months. Our results highlight the potential of ultraflexible and free-standing carbon nanofilms for stable neural interfacing in the brain.

Flexible and highly responsive photodetectors based on heterostructures of MoS2and all-carbon transistors.

Heterostructures of graphene and transition-metal dichalcogenides (TMDCs) are promising candidates for high-performance flexible photodetectors because of their high photoresponsivity and detectivity. However, the mechanical stability of current flexible photodetectors is limited, due to a mechanical mismatch between their two-dimensional channel materials and metallic contacts. Herein, we develop a type of mechanically stable, highly responsive, and flexible photodetector by integrating MoS2and all-carbon transistors. By combining the high mobility of graphene with the strong light-matter interactions of MoS2, our heterostructure photodetector exhibits a greatly improved photoresponse performance, compared with individual graphene or MoS2photodetectors. In addition, the mechanical properties of the all-carbon electrodes are a good match for those of the active two-dimensional channels, resulting in greatly improved electrical stability of the heterostructure photodetector under mechanical deformation. These capabilities make our heterostructure photodetector a promising candidate for flexible photodetection and photoimaging applications.

Carbon nanotube spiderweb promoted growth of hierarchical transition metal dichalcogenide nanostructures for seamless devices.

Hierarchical transition metal dichalcogenide (h-TMDC) nanostructures with abundant active edge sites and good electrical conductivity hold great promise for numerous applications. Here, we report a general method for the chemical synthesis of a series of large-area, free-standing h-TMDC films and their devices by using carbon nanotube (CNT) spiderwebs as both growth promoters and electrical/mechanical reinforcement networks. Our approach allows the seamless integration of h-TMDC nanostructures with abundant active edge sites and CNT networks with good electrical conductivity and mechanical flexibility. As a proof of concept, h-MoSe2/CNT hybrid films with CNT contacts have been chemically synthesized and applied as flexible electrocatalytic devices for hydrogen evolution reaction (HER). Owing to the seamless connection between the CNT contacts and the electroactive h-TMDC/CNT nanostructures, the flexible electrocatalytic devices exhibited excellent mechanical stability and maintained stable electrocatalytic performance under cyclic bendings. Our method can be readily extended to the large-scale production of various h-TMDC/CNT hybrid films and their seamless devices.

Flexible Micropillar Electrode Arrays for In Vivo Neural Activity Recordings.

Flexible electronics that can form tight interfaces with neural tissues hold great promise for improving the diagnosis and treatment of neurological disorders and advancing brain/machine interfaces. Here, the facile fabrication of a novel flexible micropillar electrode array (µPEA) is described based on a biotemplate method. The flexible and compliant µPEA can readily integrate with the soft surface of a rat cerebral cortex. Moreover, the recording sites of the µPEA consist of protruding micropillars with nanoscale surface roughness that ensure tight interfacing and efficient electrical coupling with the nervous system. As a result, the flexible µPEA allows for in vivo multichannel recordings of epileptiform activity with a high signal-to-noise ratio of 252 ± 35. The ease of preparation, high flexibility, and biocompatibility make the µPEA an attractive tool for in vivo spatiotemporal mapping of neural activity.

Multiscale Hierarchical Design of a Flexible Piezoresistive Pressure Sensor with High Sensitivity and Wide Linearity Range.

Flexible piezoresistive pressure sensors have been attracting wide attention for applications in health monitoring and human-machine interfaces because of their simple device structure and easy-readout signals. For practical applications, flexible pressure sensors with both high sensitivity and wide linearity range are highly desirable. Herein, a simple and low-cost method for the fabrication of a flexible piezoresistive pressure sensor with a hierarchical structure over large areas is presented. The piezoresistive pressure sensor consists of arrays of microscale papillae with nanoscale roughness produced by replicating the lotus leaf's surface and spray-coating of graphene ink. Finite element analysis (FEA) shows that the hierarchical structure governs the deformation behavior and pressure distribution at the contact interface, leading to a quick and steady increase in contact area with loads. As a result, the piezoresistive pressure sensor demonstrates a high sensitivity of 1.2 kPa-1 and a wide linearity range from 0 to 25 kPa. The flexible pressure sensor is applied for sensitive monitoring of small vibrations, including wrist pulse and acoustic waves. Moreover, a piezoresistive pressure sensor array is fabricated for mapping the spatial distribution of pressure. These results highlight the potential applications of the flexible piezoresistive pressure sensor for health monitoring and electronic skin.

Sensitivity limits and scaling of bioelectronic graphene transducers.

Semiconducting nanomaterials are being intensively studied as active elements in bioelectronic devices, with the aim of improving spatial resolution. Yet, the consequences of size-reduction on fundamental noise limits, or minimum resolvable signals, and their impact on device design considerations have not been defined. Here, we address these key issues by quantifying the size-dependent performance and limiting factors of graphene (Gra) transducers under physiological conditions. We show that suspended Gra devices represent the optimal configuration for cardiac extracellular electrophysiology in terms of both transducer sensitivity, systematically ~5× higher than substrate-supported devices, and forming tight bioelectronic interfaces. Significantly, noise measurements on free-standing Gra together with theoretical calculations yield a direct relationship between low-frequency 1/f noise and water dipole-induced disorders, which sets fundamental sensitivity limits for Gra devices in physiological media. As a consequence, a square-root-of-area scaling of Gra transducer sensitivity was experimentally revealed to provide a critical design rule for their implementation in bioelectronics.

Colloidal antireflection coating improves graphene-silicon solar cells.

Carbon nanotube-Si and graphene-Si solar cells have attracted much interest recently owing to their potential in simplifying manufacturing process and lowering cost compared to Si cells. Until now, the power conversion efficiency of graphene-Si cells remains under 10% and well below that of the nanotube-Si counterpart. Here, we involved a colloidal antireflection coating onto a monolayer graphene-Si solar cell and enhanced the cell efficiency to 14.5% under standard illumination (air mass 1.5, 100 mW/cm(2)) with a stable antireflection effect over long time. The antireflection treatment was realized by a simple spin-coating process, which significantly increased the short-circuit current density and the incident photon-to-electron conversion efficiency to about 90% across the visible range. Our results demonstrate a great promise in developing high-efficiency graphene-Si solar cells in parallel to the more extensively studied carbon nanotube-Si structures.

Recent developments in multifunctional neural probes for simultaneous neural recording and modulation.

Neural probes are among the most widely applied tools for studying neural circuit functions and treating neurological disorders. Given the complexity of the nervous system, it is highly desirable to monitor and modulate neural activities simultaneously at the cellular scale. In this review, we provide an overview of recent developments in multifunctional neural probes that allow simultaneous neural activity recording and modulation through different modalities, including chemical, electrical, and optical stimulation. We will focus on the material and structural design of multifunctional neural probes and their interfaces with neural tissues. Finally, future challenges and prospects of multifunctional neural probes will be discussed.

Polymer nanofiber network reinforced gold electrode array for neural activity recording.

Flexible and stretchable neural electrodes are promising tools for high-fidelity interfacing with soft and curvilinear brain surface. Here, we describe a flexible and stretchable neural electrode array that consists of polyacrylonitrile (PAN) nanofiber network reinforced gold (Au) film electrodes. Under stretching, the interweaving PAN nanofibers effectively terminate the formation of propagating cracks in the Au films and thus enable the formation of a dynamically stable electrode-tissue interface. Moreover, the PAN nanofibers increase the surface roughness and active surface areas of the Au electrodes, leading to reduced electrochemical impedance and improved signal-to-noise ratio. As a result, PAN nanofiber network reinforced Au electrode arrays can allow for reliable in vivo multichannel recording of epileptiform activities in rats. Supplementary Information: The online version contains supplementary material available at 10.1007/s13534-022-00257-5.

Free-Standing Nanofilm Electrode Arrays for Long-Term Stable Neural Interfacings.

Flexible neural electrodes integrated on micrometer-thick polymer substrates offer important opportunities for improving the stability of neuronal activity recordings during cognitive processes. However, the bending stiffness of micrometer-thick polymer substrates is typically two orders of magnitude higher than that of nanofilm electrodes, making it a limiting factor in electrode-tissue interfacings. Here, this limitation is overcome by developing self-assembled nanofilm electrode arrays (NEAs) that consist of high-density, free-standing gold nanofilm electrodes. Chronically implanted NEAs can form intimate and innervated interfaces with neural tissue, enabling stable neuronal activity recordings across multiple brain regions over several months. As an application example, the activities of the same neuronal populations are tracked across odor discrimination reversal learning and it is illustrated how dorsal striatal neurons represent and update stimulus-outcome associations across multiple timescales. The results underscore the potential of free-standing nanoscale materials for interfacing biological systems over long terms.

Flexible and Stable Carbon Nanotube Film Strain Sensors with Self-Derived Integrated Electrodes.

The development of flexible and wearable electronic devices has put an increasing demand on electrode systems with seamless connection and high compatibility with the main device, in order to accommodate complex deformation conditions and maintain stable performance. Here, we present a carbon nanotube-integrated electrode (CNTIE) by wet-pulling the ends of a carbon nanotube (CNT) film to form condensed thin fibers that resemble conventional conducting wire electrodes. A flexible strain sensor was constructed consisting of the middle CNT film as the main functional part and the CNTIE as self-derived electrodes, with inherent CNT connection between the two parts. The sensor can be transferred to versatile substrates (e.g., balloon surface) or encapsulated in thermoplastic polymers, exhibiting a large linear response range (up to 1000% in tensile strain), excellent durability and repeatability over 5000 cycles, and the ability to detect small- to large-degree human body motions. In addition, the strain sensor based on the CNTIE hybrid film (MXene/CNT and graphene/CNT) also shows superior linearity and stability at a strain range of 0-800%. Compared with the sensors using traditional silver wire electrodes and separately fabricated CNT fiber electrodes, our CNTIE plays an important role in achieving highly stable performance in the strain cycles. Our self-derived integrated electrodes provide a potential route to solve the incompatibility issues of conventional electrodes and to develop high-performance flexible and wearable systems based on CNTs and other nanomaterials.

Anti-fouling peptide functionalization of ultraflexible neural probes for long-term neural activity recordings in the brain.

Implantable neural probes constitute an essential tool for neuronal activity recordings in basic neuroscience and also hold great promise for the development of neuroprosthesis to restore lost motor or sensory functions of the body. However, conventional neural probes are susceptible to biofouling because of their physicochemical mismatch with neural tissues, resulting in signal degradation in chronic studies. Here, we describe an ultraflexible neural probe (uFNP) with anti-fouling zwitterionic peptide modification for long-term stable neural activity recordings. The anti-fouling zwitterionic peptide consists of two parts: negatively charged glutamic acid (E) and positively charged lysine (K) formed EKEKEK (EK) head to create a hydration layer that resists protein adsorption on the microelectrodes, and a fragment of laminin formed IKVAV tail to increase the adhesion of the microelectrodes to neuronal cells. We demonstrate that EK-IKVAV modified uFNPs can allow for stable neuronal activity recordings over 16 weeks. Immunohistological studies confirm that EK-IKVAV functionalized uFNPs could induce greatly reduced neuronal cell loss. Collectively, these results suggest that the anti-fouling zwitterionic peptide functionalization of uFNPs provide a promising route to construct biocompatible and stable neural interfaces.

Bioinspired flexible electronics for seamless neural interfacing and chronic recording.

Implantable neural probes are among the most widely applied tools for the understanding of neural circuit functions and the treatment of neurological disorders. Despite remarkable progress in recent years, it is still challenging for conventional rigid probes to achieve stable neural recording over long periods of time. Recently, flexible electronics with biomimetic structures and mechanical properties have been demonstrated for the formation of seamless probe-neural interfaces, enabling long-term recording stability. In this review, we provide an overview of bioinspired flexible electronics, from their structural design to probe-brain interfaces and chronic neural recording applications. Opportunities of bioinspired flexible electronics in fundamental neuroscience and clinical studies are also discussed.

Highly Transparent, Highly Thermally Stable Nanocellulose/Polymer Hybrid Substrates for Flexible OLED Devices.

Flexible organic light-emitting diode (OLED) devices based on polymer substrates have attracted worldwide attention. However, the current OLED polymer substrates are limited due to weak thermal stability, which is not compatible with the high temperature in OLED fabrication. Here, we developed a novel nanocellulose/polyarylate (PAR) hybrid polymer substrate with both high transparency and excellent thermal properties. Benefiting from the nanometer scale of the cellulose nanofibrils (CNFs) and the efficient interfacial interaction with PAR, the substrate exhibited greatly improved thermal stability, with a glass transition temperature of 192 °C, the thermal decomposition temperature of 501 °C, and upper operating temperature up to over 220 °C. Meanwhile, the hybrid substrate exhibits outstanding mechanical properties. Notably, no apparent transparency loss was observed after the CNF addition, and the hybrid substrate maintains a high transmittance of 85% and a low haze of 1.75%@600 nm. Moreover, OLED devices fabricated on the hybrid substrates exhibit a much improved optoelectrical performance than that of the devices fabricated on the conventional poly(ethylene terephthalate) (PET) substrates. We anticipate this research will open up a new route for fabricating flexible high-performance OLEDs.

Binary Thiol-Capped Gold Nanoparticle Monolayer Films for Quantitative Surface-Enhanced Raman Scattering Analysis.

Surface-enhanced Raman scattering (SERS) can provide fingerprint information of analyte molecules with unparalleled sensitivity. However, quantitative analysis using SERS has remained one of the major challenges owing to the difficulty of obtaining reproducible SERS substrates with high-density hotspots. Here, we report the rational design and fabrication of a binary thiol-capped gold nanoparticle (AuNP) monolayer film (MLF) as a substrate for highly sensitive and quantitative SERS analysis. The two thiol ligands chemically bonded to the AuNPs play different roles: dodecanethiol with a long alkyl chain controls the interparticle gaps and electromagnetic coupling among AuNPs and 4-mercaptopyridine works as a Raman internal standard (IS). The binary thiol-capped AuNPs can self-assemble into an ordered MLF with high-density hotspots and uniformly distributed IS. The as-prepared MLF has been demonstrated as a reliable SERS substrate for quantitative detection of fungicide malachite green in aqueous solution, with a high enhancement factor (up to 3.3 × 107) and a low detection limit (100 pM). Moreover, the MLF SERS substrate is flexible and transparent, which has enabled in situ detection of trace fungicide residues in a shrimp tissue.

One-Step, Catalyst-Free, Scalable in Situ Synthesis of Single-Crystal Aluminum Nanowires in Confined Graphene Space.

Nanowires have a wide range of applications, such as transparent electrodes, Li-ion battery anodes, light-emitting diodes, solar cells, and electronic devices. Currently, aluminum (Al) nanowires can be synthesized by thermally induced substitution of germanium (Ge) nanowires, chemical vapor deposition on other metal substrates, and template-assisted growth methods. However, there are still challenges in fabricating extremely high-purity nanowires, large-scale manufacturing, and simplifying the synthesis process and conditions. Here, we report for the first time that single-crystal Al nanowires can be one-step, in situ synthesized on a reduced graphene oxide (RGO) substrate on a large scale without using any catalysts. Through a simple high temperature treatment process, commercial micro-sized Al powders in RGO film were transformed into a single-crystal Al nanowire with an average length of 1.2 µm and an average diameter of 18 nm. The possible formation mechanism of the single-crystal Al nanowires is proposed as follows: hot aluminum atoms eject from the pristine aluminum/alumina core/shell structure of Al powders when they build up enough energy from the thermal stress under high temperature and confined space conditions, which is supported by both experimental and computational results. The method introduced here can be extended to allow the synthesis of one-dimensional highly reactive materials, like alkali metal nanowires, in confined spaces.

Corrigendum: Soft and wrinkled carbon membranes derived from petals for flexible supercapacitors.

This corrects the article DOI: 10.1038/srep45378.

A General Method for the Chemical Synthesis of Large-Scale, Seamless Transition Metal Dichalcogenide Electronics.

The capability to directly build atomically thin transition metal dichalcogenide (TMD) devices by chemical synthesis offers important opportunities to achieve large-scale electronics and optoelectronics with seamless interfaces. Here, a general approach for the chemical synthesis of a variety of TMD (e.g., MoS2 , WS2 , and MoSe2 ) device arrays over large areas is reported. During chemical vapor deposition, semiconducting TMD channels and metallic TMD/carbon nanotube (CNT) hybrid electrodes are simultaneously formed on CNT-patterned substrate, and then coalesce into seamless devices. Chemically synthesized TMD devices exhibit attractive electrical and mechanical properties. It is demonstrated that chemically synthesized MoS2 -MoS2 /CNT devices have Ohmic contacts between MoS2 /CNT hybrid electrodes and MoS2 channels. In addition, MoS2 -MoS2 /CNT devices show greatly enhanced mechanical stability and photoresponsivity compared with conventional gold-contacted devices, which makes them suitable for flexible optoelectronics. Accordingly, a highly flexible pixel array based on chemically synthesized MoS2 -MoS2 /CNT photodetectors is applied for image sensing.

Soft and wrinkled carbon membranes derived from petals for flexible supercapacitors.

Biomass materials are promising precursors for the production of carbonaceous materials due to their abundance, low cost and renewability. Here, a freestanding wrinkled carbon membrane (WCM) electrode material for flexible supercapacitors (SCs) was obtained from flower petal. The carbon membrane was fabricated by a simple thermal pyrolysis process and further activated by heating the sample in air. As a binder and current collector-free electrode, the activated wrinkled carbon membrane (AWCM) exhibited a high specific capacitance of 332.7 F/g and excellent cycling performance with 92.3% capacitance retention over 10000 cycles. Moreover, a flexible all-solid supercapacitor with AWCM electrode was fabricated and showed a maximum specific capacitance of 154 F/g and great bending stability. The development of this flower petal based carbon membrane provides a promising cost-effective and environmental benign electrode material for flexible energy storage.