Soft Sensors and Actuators for Wearable Human-Machine Interfaces.

Haptic human-machine interfaces (HHMIs) combine tactile sensation and haptic feedback to allow humans to interact closely with machines and robots, providing immersive experiences and convenient lifestyles. Significant progress has been made in developing wearable sensors that accurately detect physical and electrophysiological stimuli with improved softness, functionality, reliability, and selectivity. In addition, soft actuating systems have been developed to provide high-quality haptic feedback by precisely controlling force, displacement, frequency, and spatial resolution. In this Review, we discuss the latest technological advances of soft sensors and actuators for the demonstration of wearable HHMIs. We particularly focus on highlighting material and structural approaches that enable desired sensing and feedback properties necessary for effective wearable HHMIs. Furthermore, promising practical applications of current HHMI technology in various areas such as the metaverse, robotics, and user-interactive devices are discussed in detail. Finally, this Review further concludes by discussing the outlook for next-generation HHMI technology.

Hyper-Branched Gold Nanoconstructs for Photoacoustic Imaging in the Near-Infrared Optical Window.

In plasmonic nanoconstructs (NCs), fine-tuning interparticle interactions at the subnanoscale offer enhanced electromagnetic and thermal responses in the near-infrared (NIR) wavelength range. Due to tunable electromagnetic and thermal characteristics, NCs can be excellent photoacoustic (PA) imaging contrast agents. However, engineering plasmonic NCs that maximize light absorption efficiency across multiple polarization directions, i.e., exhibiting blackbody absorption behavior, remains challenging. Herein, we present the synthesis, computational simulation, and characterization of hyper-branched gold nanoconstructs (HBGNCs) as a highly efficient PA contrast agent. HBGNCs exhibit remarkable optical properties, including strong NIR absorption, high absorption efficiency across various polarization angles, and superior photostability compared to conventional standard plasmonic NC-based contrast agents such as gold nanorods and gold nanostars. In vitro and in vivo experiments confirm the suitability of HBGNCs for cancer imaging, showcasing their potential as reliable PA contrast agents and addressing the need for enhanced imaging contrast and stability in bioimaging applications.

Photoacoustic-guided ultrasound thermal imaging without prior knowledge of tissue composition.

Thermal strain imaging (TSI) is a widely investigated ultrasound (US) thermometry technique that is based on the temperature-dependent change in speed of sound. However, a major challenge of TSI is a calibration process to account for material-dependent thermal strain. In this study, we leverage nanoparticle (NP)-mediated photoacoustic (PA) thermometry to calibrate thermal strain and guide US thermal imaging. By controlling the molecular composition of the sub-micrometer layer surrounding the NPs, PA thermometry becomes independent of the thermal characteristics of the overall background tissue where the NPs reside. Thus accurate temperature measurements are obtainable from sparse NP-mediated PA signals. These measurements are used to guide TSI, allowing US thermometry to produce an expanded temperature map over the entire region of interest without prior knowledge of tissue composition. Our feasibility study in tissue-mimicking phantoms demonstrates the potential to improve TSI by integrating a PA-based calibration method that complements and guides US thermometry.

pH-responsive ratiometric photoacoustic imaging of polyaniline nanoparticle-coated needle for targeted cancer biopsy.

Cancer microenvironment exhibits lower pH compared to healthy tissues, a characteristic which can be exploited using a pH-responsive needle to increase the accuracy of cancer biopsy. A needle, coated with pH-responsive polyaniline (PANI) nanoparticles (PANI-needle), is developed for the minimally invasive and quantitative pH analysis of tissue based on ratiometric photoacoustic (PA) imaging. The ratiometric PA signal from the PANI-needle within the 850-700 nm wavelength range shows a linear response as pH changes from 7.5 to 6.5. Owing to the high surface area of nanostructured PANI, the PA signal of PANI-needle exhibits a fast and reversible response of less than a few seconds. In a tissue-mimicking hydrogel phantom composed of two regions with different pH, PA ratios of PANI-needle successfully differentiate the local pH. The PANI-needle coupled with ultrasound-guided PA imaging is a promising technology for detection of malignant tissue through quantitative pH analysis during needle biopsy.

Photosensitive ion channels in layered MXene membranes modified with plasmonic gold nanostars and cellulose nanofibers.

Ion channels transduce external stimuli into ion-transport-mediated signaling, which has received considerable attention in diverse fields such as sensors, energy harvesting devices, and desalination membrane. In this work, we present a photosensitive ion channel based on plasmonic gold nanostars (AuNSs) and cellulose nanofibers (CNFs) embedded in layered MXene nanosheets. The MXene/AuNS/CNF (MAC) membrane provides subnanometer-sized ionic pathways for light-sensitive cationic flow. When the MAC nanochannel is exposed to NIR light, a photothermal gradient is formed, which induces directional photothermo-osmotic flow of nanoconfined electrolyte against the thermal gradient and produces a net ionic current. MAC membrane exhibits enhanced photothermal current compared with pristine MXene, which is attributed to the combined photothermal effects of plasmonic AuNSs and MXene and the widened interspacing of the MAC composite via the hydrophilic nanofibrils. The MAC composite membranes are envisioned to be applied in flexible ionic channels with ionogels and light-controlled ionic circuits.

Tunable Interparticle Connectivity in Gold Nanosphere Assemblies for Efficient Photoacoustic Conversion.

Manipulating matter at the nanometer scale to create desired plasmonic nanostructures holds great promise in the field of biomedical photoacoustic (PA) imaging. We demonstrate a strategy for regulating PA signal generation from anisotropic nano-sized assemblies of gold nanospheres (Au NSs) by adjusting the inter-particle connectivity between neighboring Au NSs. The inter-particle connectivity is controlled by modulating the diameter and inter-particle spacing of Au NSs in the nanoassemblies. The results indicate that nanoassemblies with semi-connectivity, i.e., assemblies with a finite inter-particle spacing shorter than the theoretical limit of repulsion between nearby Au NSs, exhibit 3.4-fold and 2.4-fold higher PA signals compared to nanoassemblies with no connectivity and full connectivity, respectively. Furthermore, due to the reduced diffusion of Au atoms, the semi-connectivity Au nanoassemblies demonstrate high photodamage threshold and, therefore, excellent photostability at fluences above the current American National Standards Institute limits. The exceptional photostability of the semi-connectivity nanoassemblies highlights their potential to surpass conventional plasmonic contrast agents for continuing PA imaging. Collectively, our findings indicate that semi-connected nanostructures are a promising option for reliable, high-contrast PA imaging applications over multiple imaging sessions due to their strong PA signals and enhanced photostability.

Adaptive IR- and Water-Gating Textiles Based on Shape Memory Fibers.

Thermoregulation is an essential function of the human body for adapting to the surrounding temperature. Stimuli-responsive smart textiles can provide effective protection of the human skin temperature from a continuously changing environment. Herein, we develop a smart textile based on shape memory polymer (SMP) fibers for adaptive regulation of IR and water transmission on human skin. An SMP textile is fabricated with hierarchical micro/nanoporous structures to enhance thermal insulation performance, and silver nanowires are coated on one side to provide asymmetric IR reflectivity and hydrophilicity. The porous SMP textile shows great tunability of thermal insulation and asymmetric wettability by deformation and recovery of the shape and structure in response to stimuli. The degree of thermal insulation is controlled by 65.7% of the original value, and the surface temperature of the SMP textile on a hot plate is successfully controlled in the IR images due to adaptive IR reflectivity. Additionally, the directional transportation of water droplets can be switched on/off according to the shape of the SMP textiles, which can be employed for sweat removal from the human skin. This IR- and water-gating smart textile can provide a feasible strategy for protecting the human skin from external environmental changes.

Flexible Pyroresistive Graphene Composites for Artificial Thermosensation Differentiating Materials and Solvent Types.

When we touch an object, thermosensation allows us to perceive not only the temperature but also wetness and types of materials with different thermophysical properties (i.e., thermal conductivity and heat capacity) of objects. Emulation of such sensory abilities is important in robots, wearables, and haptic interfaces, but it is challenging because they are not directly perceptible sensations but rather learned abilities via sensory experiences. Emulating the thermosensation of human skin, we introduce an artificial thermosensation based on an intelligent thermo-/calorimeter (TCM) that can objectively differentiate types of contact materials and solvents with different thermophysical properties. We demonstrate a TCM based on pyroresistive composites with ultrahigh sensitivity (11.2% °C-1) and high accuracy (<0.1 °C) by precisely controlling the melt-induced volume expansion of a semicrystalline polymer, as well as the negative temperature coefficient of reduced graphene oxide. In addition, the ultrathin TCM with coplanar electrode design shows deformation-insensitive temperature sensing, facilitating wearable skin temperature monitoring with accuracy higher than a commercial thermometer. Moreover, the TCM with a high pyroresistivity can objectively differentiate types of contact materials and solvents with different thermophysical properties. In a proof-of-principle application, our intelligent TCM, coupled with a machine-learning algorithm, enables objective evaluation of the thermal attributes (coolness and wetness) of skincare products.

Highly Transparent, Flexible, and Self-Healable Thermoacoustic Loudspeakers.

Thermoacoustic (TA) loudspeakers have garnered significant attention in recent times as a novel film speaker that utilizes temperature oscillation to vibrate the surrounding air. Conventional film-type TA loudspeakers are known to experience problems when external environments damage their conductive networks, causing them to malfunction. Therefore, introducing self-healing polymers in TA loudspeakers could be an effective way to restore the surface damage of conductive networks. In this study, we present transparent, flexible, and self-healable TA loudspeakers based on silver nanowire (AgNW)-poly(urethane-hindered urea) (PUHU) conductive electrodes. Our self-healable AgNW/PUHU electrodes exhibit significant self-healing for repairing the surface damages that are caused due to the dynamic reconstruction of reversible bulky urea bonds in PUHU. The fabricated self-healable TA loudspeakers generate a sound pressure level of 61 dB at 10 kHz frequency (alternating current (AC) 7 V/direct current (DC) 1 V). In particular, the TA speakers are able to recover the original sound after healing the surface damages of electrodes at 95 °C and 80% relative humidity within 5 min. We believe that the technique proposed in this study provides a robust and powerful platform for the fabrication of transparent and flexible TA loudspeakers with excellent self-healing, which can be applied in flexible and wearable acoustic electronics.

Soft and ion-conducting hydrogel artificial tongue for astringency perception.

Artificial tongues have been receiving increasing attention for the perception of five basic tastes. However, it is still challenging to fully mimic human tongue-like performance for tastes such as astringency. Mimicking the mechanism of astringency perception on the human tongue, we use a saliva-like chemiresistive ionic hydrogel anchored to a flexible substrate as a soft artificial tongue. When exposed to astringent compounds, hydrophobic aggregates form inside the microporous network and transform it into a micro/nanoporous structure with enhanced ionic conductivity. This unique human tongue-like performance enables tannic acid to be detected over a wide range (0.0005 to 1 wt %) with high sensitivity (0.292 wt %-1) and fast response time (~10 s). As a proof of concept, our sensor can detect the degree of astringency in beverages and fruits using a simple wipe-and-detection method, making a powerful platform for future applications involving humanoid robots and taste monitoring devices.

Lithography-Free Route to Hierarchical Structuring of High-χ Block Copolymers on a Gradient Patterned Surface.

A chemically defined patterned surface was created via a combined process of controlled evaporative self-assembly of concentric polymer stripes and the selective surface modification of polymer brush. The former process involved physical adsorption of poly (methyl methacrylate) (PMMA) segments into silicon oxide surface, thus forming ultrathin PMMA stripes, whereas the latter process was based on the brush treatment of silicon native oxide surface using a hydroxyl-terminated polystyrene (PS-OH). The resulting alternating PMMA- and PS-rich stripes provided energetically favorable regions for self-assembly of high χ polystyrene-block-polydimethylsiloxane (PS-b-PDMS) in a simple and facile manner, dispensing the need for conventional lithography techniques. Subsequently, deep reactive ion etching and oxygen plasma treatment enabled the transition of the PDMS blocks into oxidized groove-shaped nanostructures.

Nanoparticle-Enhanced Silver-Nanowire Plasmonic Electrodes for High-Performance Organic Optoelectronic Devices.

Improved performance in plasmonic organic solar cells (OSCs) and organic light-emitting diodes (OLEDs) via strong plasmon-coupling effects generated by aligned silver nanowire (AgNW) transparent electrodes decorated with core-shell silver-silica nanoparticles (Ag@SiO2 NPs) is demonstrated. NP-enhanced plasmonic AgNW (Ag@SiO2 NP-AgNW) electrodes enable substantially enhanced radiative emission and light absorption efficiency due to strong hybridized plasmon coupling between localized surface plasmons (LSPs) and propagating surface plasmon polaritons (SPPs) modes, which leads to improved device performance in organic optoelectronic devices (OODs). The discrete dipole approximation (DDA) calculation of the electric field verifies a strongly enhanced plasmon-coupling effect caused by decorating core-shell Ag@SiO2 NPs onto the AgNWs. Notably, an electroluminescence efficiency of 25.33 cd A-1 (at 3.2 V) and a power efficiency of 25.14 lm W-1 (3.0 V) in OLEDs, as well as a power conversion efficiency (PCE) value of 9.19% in OSCs are achieved using hybrid Ag@SiO2 NP-AgNW films. These are the highest values reported to date for optoelectronic devices based on AgNW electrodes. This work provides a new design platform to fabricate high-performance OODs, which can be further explored in various plasmonic and optoelectronic devices.

Particle-Film Plasmons on Periodic Silver Film over Nanosphere (AgFON): A Hybrid Plasmonic Nanoarchitecture for Surface-Enhanced Raman Spectroscopy.

Plasmonic systems based on particle-film plasmonic couplings have recently attracted great attention because of the significantly enhanced electric field at the particle-film gaps. Here, we introduce a hybrid plasmonic architecture utilizing combined plasmonic effects of particle-film gap plasmons and silver film over nanosphere (AgFON) substrates. When gold nanoparticles (AuNPs) are assembled on AgFON substrates with controllable particle-film gap distances, the AuNP-AgFON system supports multiple plasmonic couplings from interparticle, particle-film, and crevice gaps, resulting in a huge surface-enhanced Raman spectroscopy (SERS) effect. We show that the periodicity of AgFON substrates and the particle-film gaps greatly affects the surface plasmon resonances, and thus, the SERS effects due to the interplay between multiple plasmonic couplings. The optimally designed AuNP-AgFON substrate shows a SERS enhancement of 233 times compared to the bare AgFON substrate. The ultrasensitive SERS sensing capability is also demonstrated by detecting glutathione, a neurochemical molecule that is an important antioxidant, down to the 10 pM level.

Capillary Printing of Highly Aligned Silver Nanowire Transparent Electrodes for High-Performance Optoelectronic Devices.

Percolation networks of silver nanowires (AgNWs) are commonly used as transparent conductive electrodes (TCEs) for a variety of optoelectronic applications, but there have been no attempts to precisely control the percolation networks of AgNWs that critically affect the performances of TCEs. Here, we introduce a capillary printing technique to precisely control the NW alignment and the percolation behavior of AgNW networks. Notably, partially aligned AgNW networks exhibit a greatly lower percolation threshold, which leads to the substantial improvement of optical transmittance (96.7%) at a similar sheet resistance (19.5 Ω sq(-1)) as compared to random AgNW networks (92.9%, 20 Ω sq(-1)). Polymer light-emitting diodes (PLEDs) using aligned AgNW electrodes show a 30% enhanced maximum luminance (33068 cd m(-2)) compared to that with random AgNWs and a high luminance efficiency (14.25 cd A(-1)), which is the highest value reported so far using indium-free transparent electrodes for fluorescent PLEDs. In addition, polymer solar cells (PSCs) using aligned AgNW electrodes exhibit a power conversion efficiency (PCE) of 8.57%, the highest value ever reported to date for PSCs using AgNW electrodes.