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.

Evidence for moiré excitons in van der Waals heterostructures.

Recent advances in the isolation and stacking of monolayers of van der Waals materials have provided approaches for the preparation of quantum materials in the ultimate two-dimensional limit1,2. In van der Waals heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice3. It is widely recognized that the moiré superlattice can modulate the electronic band structure of the material and lead to transport properties such as unconventional superconductivity4 and insulating behaviour driven by correlations5-7; however, the influence of the moiré superlattice on optical properties has not been investigated experimentally. Here we report the observation of multiple interlayer exciton resonances with either positive or negative circularly polarized emission in a molybdenum diselenide/tungsten diselenide (MoSe2/WSe2) heterobilayer with a small twist angle. We attribute these resonances to excitonic ground and excited states confined within the moiré potential. This interpretation is supported by recombination dynamics and by the dependence of these interlayer exciton resonances on twist angle and temperature. These results suggest the feasibility of engineering artificial excitonic crystals using van der Waals heterostructures for nanophotonics and quantum information applications.

Effects of AC frequency on the capacitance measurement of hybrid response pressure sensors.

E-skins consisting of soft pressure sensors are enabling technology for soft robots, bio-integrated devices, and deformable touch panels. A well-known bottleneck of capacitive pressure sensors (CPS) is the drastic decay in sensitivity with increasing pressure. To overcome this challenge, we have invented a hybrid-response pressure sensor (HRPS) that exhibits both the piezoresistive and piezocapacitive effects intrinsic to a highly porous nanocomposite (PNC) with carbon nanotube (CNT) dopants. The HRPS is constructed with two conductive electrodes sandwiching a laminated PNC and a stiff dielectric layer. We have simplified the hybrid response into a parallel resistor-capacitor circuit, whose output depends on the AC (alternating current) frequency used for the capacitance measurement. Herein, through theoretical analysis, we discover a dimensionless parameter that governs the frequency responses of the HRPS. The master curve is validated through experiments on the HRPS with various doping ratios, subject to different compressive strains, under diverse AC frequencies. In addition, the relative contribution of piezoresistive and piezocapacitive mechanisms are also found to vary with the three parameters. Based on this experimentally validated theory, we establish a very practical guideline for selecting the optimal AC frequency for the capacitance measurement of HRPSs.

Mechanics of spontaneously formed nanoblisters trapped by transferred 2D crystals.

Layered systems of 2D crystals and heterostructures are widely explored for new physics and devices. In many cases, monolayer or few-layer 2D crystals are transferred to a target substrate including other 2D crystals, and nanometer-scale blisters form spontaneously between the 2D crystal and its substrate. Such nanoblisters are often recognized as an indicator of good adhesion, but there is no consensus on the contents inside the blisters. While gas-filled blisters have been modeled and measured by bulge tests, applying such models to spontaneously formed nanoblisters yielded unrealistically low adhesion energy values between the 2D crystal and its substrate. Typically, gas-filled blisters are fully deflated within hours or days. In contrast, we found that the height of the spontaneously formed nanoblisters dropped only by 20-30% after 3 mo, indicating that probably liquid instead of gas is trapped in them. We therefore developed a simple scaling law and a rigorous theoretical model for liquid-filled nanoblisters, which predicts that the interfacial work of adhesion is related to the fourth power of the aspect ratio of the nanoblister and depends on the surface tension of the liquid. Our model was verified by molecular dynamics simulations, and the adhesion energy values obtained for the measured nanoblisters are in good agreement with those reported in the literature. This model can be applied to estimate the pressure inside the nanoblisters and the work of adhesion for a variety of 2D interfaces, which provides important implications for the fabrication and deformability of 2D heterostructures and devices.

Interface-Governed Deformation of Nanobubbles and Nanotents Formed by Two-Dimensional Materials.

Nanoblisters such as nanobubbles and nanotents formed by two-dimensional (2D) materials have been extensively exploited for strain engineering purposes as they can produce self-sustained, nonuniform in-plane strains through out-of-plane deformation. However, deterministic measure and control of strain fields in these systems are challenging because of the atomic thinness and unconventional interface behaviors of 2D materials. Here, we experimentally characterize a simple and unified power law for the profiles of a variety of nanobubbles and nanotents formed by 2D materials such as graphene and MoS_{2} layers. Using membrane theory, we analytically unveil what sets the in-plane strains of these blisters regarding their shape and interface characteristics. Our analytical solutions are validated by Raman spectroscopy measured strain distributions in bulged graphene bubbles supported by strong and weak shear interfaces. We advocate that both the strain magnitudes and distributions can be tuned by 2D material-substrate interface adhesion and friction properties.

Suction effects of craters under water.

Octopus-inspired cratered surfaces have recently emerged as a new class of reusable physical adhesives. Preload-dependent adhesion and enhanced adhesion under water distinguish them from the well-studied gecko-inspired pillared surfaces. Despite growing experimental evidence, modeling frameworks and mechanistic understanding of cratered surfaces are still very limited. We recently developed a framework to evaluate suction forces produced by isolated craters in air. In this paper, we focus on underwater craters. The suction force-preload relation predicted by this framework has been validated by experiments carried out with an incompressible fluid under small and moderate preloads. Our model breaks down under a large preload due to multiple possible reasons including liquid vaporization. A direct comparison between liquid and air-filled craters has been carried out and the dependence on the depth of water has been revealed. We find that the suction forces generated by underwater craters scale with the specimen modulus but exhibit non-monotonic dependence on the aspect ratio of the craters.

Assessment of Dry Epidermal Electrodes for Long-Term Electromyography Measurements.

Commercially available electrodes can only provide quality surface electromyography (sEMG) measurements for a limited duration due to user discomfort and signal degradation, but in many applications, collecting sEMG data for a full day or longer is desirable to enhance clinical care. Few studies for long-term sEMG have assessed signal quality of electrodes using clinically relevant tests. The goal of this research was to evaluate flexible, gold-based epidermal sensor system (ESS) electrodes for long-term sEMG recordings. We collected sEMG and impedance data from eight subjects from ESS and standard clinical electrodes on upper extremity muscles during maximum voluntary isometric contraction tests, dynamic range of motion tests, the Jebsen Taylor Hand Function Test, and the Box & Block Test. Four additional subjects were recruited to test the stability of ESS signals over four days. Signals from the ESS and traditional electrodes were strongly correlated across tasks. Measures of signal quality, such as signal-to-noise ratio and signal-to-motion ratio, were also similar for both electrodes. Over the four-day trial, no significant decrease in signal quality was observed in the ESS electrodes, suggesting that thin, flexible electrodes may provide a robust tool that does not inhibit movement or irritate the skin for long-term measurements of muscle activity in rehabilitation and other applications.

Out-of-Plane Electromechanical Response of Monolayer Molybdenum Disulfide Measured by Piezoresponse Force Microscopy.

Two-dimensional (2D) materials have recently been theoretically predicted and experimentally confirmed to exhibit electromechanical coupling. Specifically, monolayer and few-layer molybdenum disulfide (MoS2) have been measured to be piezoelectric within the plane of their atoms. This work demonstrates and quantifies a nonzero out-of-plane electromechanical response of monolayer MoS2 and discusses its possible origins. A piezoresponse force microscope was used to measure the out-of-plane deformation of monolayer MoS2 on Au/Si and Al2O3/Si substrates. Using a vectorial background subtraction technique, we estimate the effective out-of-plane piezoelectric coefficient, d33eff, for monolayer MoS2 to be 1.03 ± 0.22 pm/V when measured on the Au/Si substrate and 1.35 ± 0.24 pm/V when measured on Al2O3/Si. This is on the same order as the in-plane coefficient d11 reported for monolayer MoS2. Interpreting the out-of-plane response as a flexoelectric response, the effective flexoelectric coefficient, µeff*, is estimated to be 0.10 nC/m. Analysis has ruled out the possibility of elastic and electrostatic forces contributing to the measured electromechanical response. X-ray photoelectron spectroscopy detected some contaminants on both MoS2 and its substrate, but the background subtraction technique is expected to remove major contributions from the unwanted contaminants. These measurements provide evidence that monolayer MoS2 exhibits an out-of-plane electromechanical response and our analysis offers estimates of the effective piezoelectric and flexoelectric coefficients.

Flexible black phosphorus ambipolar transistors, circuits and AM demodulator.

High-mobility two-dimensional (2D) semiconductors are desirable for high-performance mechanically flexible nanoelectronics. In this work, we report the first flexible black phosphorus (BP) field-effect transistors (FETs) with electron and hole mobilities superior to what has been previously achieved with other more studied flexible layered semiconducting transistors such as MoS2 and WSe2. Encapsulated bottom-gated BP ambipolar FETs on flexible polyimide afforded maximum carrier mobility of about 310 cm(2)/V·s with field-effect current modulation exceeding 3 orders of magnitude. The device ambipolar functionality and high-mobility were employed to realize essential circuits of electronic systems for flexible technology including ambipolar digital inverter, frequency doubler, and analog amplifiers featuring voltage gain higher than other reported layered semiconductor flexible amplifiers. In addition, we demonstrate the first flexible BP amplitude-modulated (AM) demodulator, an active stage useful for radio receivers, based on a single ambipolar BP transistor, which results in audible signals when connected to a loudspeaker or earphone. Moreover, the BP transistors feature mechanical robustness up to 2% uniaxial tensile strain and up to 5000 bending cycles.

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.

Brain implantation of tissue-level-soft bioelectronics via embryonic development.

The design of bioelectronics capable of stably tracking brain-wide, single-cell, and millisecond-resolved neural activities in the developing brain is critical to the study of neuroscience and neurodevelopmental disorders. During development, the three-dimensional (3D) structure of the vertebrate brain arises from a 2D neural plate 1,2 . These large morphological changes previously posed a challenge for implantable bioelectronics to track neural activity throughout brain development 3-9 . Here, we present a tissue-level-soft, sub-micrometer-thick, stretchable mesh microelectrode array capable of integrating into the embryonic neural plate of vertebrates by leveraging the 2D-to-3D reconfiguration process of the tissue itself. Driven by the expansion and folding processes of organogenesis, the stretchable mesh electrode array deforms, stretches, and distributes throughout the entire brain, fully integrating into the 3D tissue structure. Immunostaining, gene expression analysis, and behavioral testing show no discernible impact on brain development or function. The embedded electrode array enables long-term, stable, brain-wide, single-unit-single-spike-resolved electrical mapping throughout brain development, illustrating how neural electrical activities and population dynamics emerge and evolve during brain development.

3D spatiotemporally scalable in vivo neural probes based on fluorinated elastomers.

Electronic devices for recording neural activity in the nervous system need to be scalable across large spatial and temporal scales while also providing millisecond and single-cell spatiotemporal resolution. However, existing high-resolution neural recording devices cannot achieve simultaneous scalability on both spatial and temporal levels due to a trade-off between sensor density and mechanical flexibility. Here we introduce a three-dimensional (3D) stacking implantable electronic platform, based on perfluorinated dielectric elastomers and tissue-level soft multilayer electrodes, that enables spatiotemporally scalable single-cell neural electrophysiology in the nervous system. Our elastomers exhibit stable dielectric performance for over a year in physiological solutions and are 10,000 times softer than conventional plastic dielectrics. By leveraging these unique characteristics we develop the packaging of lithographed nanometre-thick electrode arrays in a 3D configuration with a cross-sectional density of 7.6 electrodes per 100 µm2. The resulting 3D integrated multilayer soft electrode array retains tissue-level flexibility, reducing chronic immune responses in mouse neural tissues, and demonstrates the ability to reliably track electrical activity in the mouse brain or spinal cord over months without disrupting animal behaviour.

Flexible and stretchable electronics for biointegrated devices.

Advances in materials, mechanics, and manufacturing now allow construction of high-quality electronics and optoelectronics in forms that can readily integrate with the soft, curvilinear, and time-dynamic surfaces of the human body. The resulting capabilities create new opportunities for studying disease states, improving surgical procedures, monitoring health/wellness, establishing human-machine interfaces, and performing other functions. This review summarizes these technologies and illustrates their use in forms integrated with the brain, the heart, and the skin.

Gauge factor and stretchability of silicon-on-polymer strain gauges.

Strain gauges are widely applied to measure mechanical deformation of structures and specimens. While metallic foil gauges usually have a gauge factor slightly over 2, single crystalline silicon demonstrates intrinsic gauge factors as high as 200. Although silicon is an intrinsically stiff and brittle material, flexible and even stretchable strain gauges have been achieved by integrating thin silicon strips on soft and deformable polymer substrates. To achieve a fundamental understanding of the large variance in gauge factor and stretchability of reported flexible/stretchable silicon-on-polymer strain gauges, finite element and analytically models are established to reveal the effects of the length of the silicon strip, and the thickness and modulus of the polymer substrate. Analytical results for two limiting cases, i.e., infinitely thick substrate and infinitely long strip, have found good agreement with FEM results. We have discovered that strains in silicon resistor can vary by orders of magnitude with different substrate materials whereas strip length or substrate thickness only affects the strain level mildly. While the average strain in silicon reflects the gauge factor, the maximum strain in silicon governs the stretchability of the system. The tradeoff between gauge factor and stretchability of silicon-on-polymer strain gauges has been proposed and discussed.

A Multi-Day Wearable Surface EMG E-Tattoo for Fatigue Monitoring.

Surface electromyography (sEMG) is a commonly used technique for the non-invasive measurement of muscle activity. However, the traditional electrodes used for sEMG often have limitations regarding their long-term wearability. This study explored the feasibility of a wearable platform using a tattoo-like epidermal electrode (e-tattoo) for multi-day sEMG monitoring. Our sEMG e-tattoo provided stable and reliable sEMG signals over three days of application comparable to conventional gel electrodes. In addition, the e-tattoo has great resistance to motion artifacts and, therefore, maintains a high signal-to-noise ratio (SNR) and signal-to-motion ratio (SMR) during dynamic activities such as cycling. This robust wearable platform opens up new avenues for developing future wearable sEMG devices and advancing dynamic muscle fatigue research.Clinical relevance- The proposed wearable sEMG system can provide continuous and non-invasive monitoring of muscle activity, providing insights for improving rehabilitation and EMG-based prosthesis development for patients.

Towards Simultaneous Noninvasive Arterial and Venous Oxygenation Monitoring with Wearable E-Tattoo.

While noninvasive arterial blood oxygenation is easily estimated using peripheral pulse oximeters, noninvasive venous blood oxygenation monitoring is still a critical unmet need. Critical conditions that lead to inefficient extraction of oxygen from the blood, such as sepsis or shock, can only be detected by analyzing the oxygen content of the venous blood. In this work, we introduce a soft wearable e-tattoo sensor that simultaneously measures the arterial and venous pulses from the wrist. First, we prove that the origin of the signal is venous pulsatility. We hypothesize that a significant obstacle for simultaneous SaO2 and SvO2 extraction is the close proximity of the artery and vein, thus leading to crosstalk. We characterize this crosstalk with simulation, in vitro, and in vivo experiments. Finally, we offer a potential solution for minimizing the crosstalk through spatial filtering.Clinical Relevance- This lays foundational work for a novel method of noninvasively and simultaneously measuring arterial and venous blood oxygenation to improve clinical diagnoses of sepsis, shock, and metabolic abnormalities.

Conformability of flexible sheets on spherical surfaces.

Three-dimensional surface-conformable electronics is a burgeoning technology with potential applications in curved displays, bioelectronics, and biomimetics. Flexible electronics are notoriously difficult to fully conform to nondevelopable surfaces such as spheres. Although stretchable electronics can well conform to nondevelopable surfaces, they need to sacrifice pixel density for stretchability. Various empirical designs have been explored to improve the conformability of flexible electronics on spherical surfaces. However, no rational design guidelines exist. This study uses a combination of experimental, analytical, and numerical approaches to systematically investigate the conformability of both intact and partially cut circular sheets on spherical surfaces. Through the analysis of thin film buckling on curved surfaces, we identify a scaling law that predicts the conformability of flexible sheets on spherical surfaces. We also quantify the effects of radial slits on enhancing conformability and provide a practical guideline for using these slits to improve conformability from 40% to more than 90%.