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.

Near-Field Electrospinning for Three-Dimensional Stacked Nanoarchitectures with High Aspect Ratios.

Near-field electrospinning (NFES) was developed to overcome the intrinsic instability of traditional electrospinning processes and to facilitate the controllable deposition of nanofibers under a reduced electric field. This technique offers a straightforward and versatile method for the precision patterning of two-dimensional (2D) nanofibers. However, three-dimensional (3D) stacked structures built by NFES have been limited to either micron-scale sizes or special shapes. Herein, we report on a direct-write 3D NFES technique to construct self-aligned, template-free, 3D stacked nanoarchitectures by simply adding salt to the polymer solution. Numerical simulations suggested that the electric field could be tuned to achieve self-aligned nanofibers by adjusting the conductivity of the polymer solution. This was confirmed experimentally by using poly(ethylene oxide) (PEO) solutions containing 0.1-1.0 wt% NaCl. Using 0.1 wt% NaCl, nanowalls with a maximum of 80 layers could be built with a width of 92 ± 3 nm, height of 6.6 ± 0.1 µm, and aspect ratio (height/width) of 72. We demonstrate the 3D printing of nanoskyscrapers with various designs, such as curved "nanowall arrays", nano "jungle gyms," and "nanobridges". Further, we present an application of the 3D stacked nanofiber arrays by preparing transparent and flexible polydimethylsiloxane films embedded with Ag-sputtered nanowalls as 3D nanoelectrodes. The conductivity of the nanoelectrodes can be precisely tuned by adjusting the number of 3D printed layers, without sacrificing transmittance (98.5%). The current NFES approach provides a simple, reliable route to build 3D stacked nanoarchitectures with high-aspect ratios for potential application in smart materials, energy devices, and biomedical applications.

Tailored Poly(vinylidene fluoride-co-trifluoroethylene) Crystal Orientation for a Triboelectric Nanogenerator through Epitaxial Growth on a Chitin Nanofiber Film.

Tailoring the crystal orientation of poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE) has attracted widespread interest because of its effects on the ferroelectric properties required for various electronic devices. In this study, we investigated the epitaxial growth of PVDF-TrFE on a chitin film for developing triboelectric nanogenerators (TENGs). The crystallographic match between the chitin and PVDF-TrFE enables the development of the intended crystal orientation, with the PVDF-TrFE polarization axis aligned perpendicular to the substrate. In addition, the epitaxially grown PVDF-TrFE on chitin not only enhances the performance of the TENG but also increases the stability of the hygroscopic chitin film against water. The corresponding TENG exhibits a significantly higher output current compared to that of a nonepitaxial PVDF-TrFE/chitin film. Furthermore, the triboelectric sensors based on epitaxial PVDF-TrFE/chitin films allow the monitoring of subtle pressures, suggesting that tailoring the crystal orientation of PVDF-TrFE is a promising approach for developing high-performance TENGs.

A Flexible High-Performance Photoimaging Device Based on Bioinspired Hierarchical Multiple-Patterned Plasmonic Nanostructures.

In insect eyes, ommatidia with hierarchical structured cornea play a critical role in amplifying and transferring visual signals to the brain through optic nerves, enabling the perception of various visual signals. Here, inspired by the structure and functions of insect ommatidia, a flexible photoimaging device is reported that can simultaneously detect and record incoming photonic signals by vertically stacking an organic photodiode and resistive memory device. A single-layered, hierarchical multiple-patterned back reflector that can exhibit various plasmonic effects is incorporated into the organic photodiode. The multiple-patterned flexible organic photodiodes exhibit greatly enhanced photoresponsivity due to the increased light absorption in comparison with the flat systems. Moreover, the flexible photoimaging device shows a well-resolved spatiotemporal mapping of optical signals with excellent operational and mechanical stabilities at low driving voltages below half of the flat systems. Theoretical calculation and scanning near-field optical microscopy analyses clearly reveal that multiple-patterned electrodes have much stronger surface plasmon coupling than flat and single-patterned systems. The developed methodology provides a versatile and effective route for realizing high-performance optoelectronic and photonic systems.

Smart Actuators and Adhesives for Reconfigurable Matter.

Biological systems found in nature provide excellent stimuli-responsive functions. The camouflage adaptation of cephalopods (octopus, cuttlefish), rapid stiffness change of sea cucumbers, opening of pine cones in response to humidity, and rapid closure of Venus flytraps upon insect touch are some examples of nature's smart systems. Although current technologies are still premature to mimic these sophisticated structures and functions in smart biological systems, recent work on stimuli-responsive programmable matter has shown great progress. Stimuli-responsive materials based on hydrogels, responsive nanocomposites, hybrid structures, shape memory polymers, and liquid crystal elastomers have demonstrated excellent responsivities to various stimuli such as temperature, light, pH, and electric field. However, the technologies in these stimuli-responsive materials are still not sophisticated enough to demonstrate the ultimate attributes of an ideal programmable matter: fast and reversible reconfiguration of programmable matter into complex and robust shapes. Recently, reconfigurable (or programmable) matter that reversibly changes its structure/shape or physical/chemical properties in response to external stimuli has attracted great interest for applications in sensors, actuators, robotics, and smart systems. In particular, key attributes of programmable matter including fast and reversible reconfiguration into complex and robust 2D and 3D shapes have been demonstrated by various approaches. In this Account, we review focused areas of smart materials with special emphasis on the material and device structure designs to enhance the response time, reversibility, multistimuli responsiveness, and smart adhesion for efficient shape transformation and functional actuations. First, the capability of fast reconfiguration of 2D and 3D structures in a reversible way is a critical requirement for programmable matter. For the fast and reversible reconfiguration, various approaches based on enhanced solvent diffusion rate through the porous or structured hydrogel materials, electrostatic repulsion between cofacial electrolyte nanosheets, and photothermal actuation are discussed. Second, the ability to reconfigure programmable matters into a variety of complex structures is beneficial for the use of reconfigurable matter in diverse applications. For the reconfiguration of planar 2D structures into complex 3D structures, asymmetric and multidirectional stress should be applied. In this regard, local hinges with stimuli-responsive stiffness, multilayer laminations with different responsiveness in individual layers, and origami and kirigami assembly approaches are reviewed. Third, multistimuli responsiveness will be required for the efficient reconfiguration of complex programmable matter in response to user-defined stimulus under different chemical and physical environments. In addition, with multistimuli responsiveness, the reconfigured shape can be temporarily affixed by one signal and disassembled by another signal at a user-defined location and time. Photoactuation depending on the chirality of carbon nanotubes and composite gels with different responsiveness will be discussed. Finally, the development of smart adhesives with on-demand adhesion strength is critically required to maintain the robust reconfigurable shapes and for the switching on/off of the binding between components or with target objects. Among various connectors and adhesives, thermoresponsive nanowire connectors, octopus-inspired smart adhesives, and elastomeric tiles with soft joints are described due to their potential applications in joints of deformable 3D structures and smart gripping systems.

A Triple-Mode Flexible E-Skin Sensor Interface for Multi-Purpose Wearable Applications.

This study presents a flexible wireless electronic skin (e-skin) sensor system that includes a multi-functional sensor device, a triple-mode reconfigurable readout integrated circuit (ROIC), and a mobile monitoring interface. The e-skin device's multi-functionality is achieved by an interlocked micro-dome array structure that uses a polyvinylidene fluoride and reduced graphene oxide (PVDF/RGO) composite material that is inspired by the structure and functions of the human fingertip. For multi-functional implementation, the proposed triple-mode ROIC is reconfigured to support piezoelectric, piezoresistance, and pyroelectric interfaces through single-type e-skin sensor devices. A flexible system prototype was developed and experimentally verified to provide various wireless wearable sensing functions-including pulse wave, voice, chewing/swallowing, breathing, knee movements, and temperature-while their real-time sensed data are displayed on a smartphone.

Ultrathin compound semiconductor on insulator layers for high-performance nanoscale transistors.

Over the past several years, the inherent scaling limitations of silicon (Si) electron devices have fuelled the exploration of alternative semiconductors, with high carrier mobility, to further enhance device performance. In particular, compound semiconductors heterogeneously integrated on Si substrates have been actively studied: such devices combine the high mobility of III-V semiconductors and the well established, low-cost processing of Si technology. This integration, however, presents significant challenges. Conventionally, heteroepitaxial growth of complex multilayers on Si has been explored-but besides complexity, high defect densities and junction leakage currents present limitations in this approach. Motivated by this challenge, here we use an epitaxial transfer method for the integration of ultrathin layers of single-crystal InAs on Si/SiO(2) substrates. As a parallel with silicon-on-insulator (SOI) technology, we use 'XOI' to represent our compound semiconductor-on-insulator platform. Through experiments and simulation, the electrical properties of InAs XOI transistors are explored, elucidating the critical role of quantum confinement in the transport properties of ultrathin XOI layers. Importantly, a high-quality InAs/dielectric interface is obtained by the use of a novel thermally grown interfacial InAsO(x) layer (~1 nm thick). The fabricated field-effect transistors exhibit a peak transconductance of ~1.6 mS µm(-1) at a drain-source voltage of 0.5 V, with an on/off current ratio of greater than 10,000.

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.

Piezoresistive Tactile Sensor Discriminating Multidirectional Forces.

Flexible tactile sensors capable of detecting the magnitude and direction of the applied force together are of great interest for application in human-interactive robots, prosthetics, and bionic arms/feet. Human skin contains excellent tactile sensing elements, mechanoreceptors, which detect their assigned tactile stimuli and transduce them into electrical signals. The transduced signals are transmitted through separated nerve fibers to the central nerve system without complicated signal processing. Inspired by the function and organization of human skin, we present a piezoresistive type tactile sensor capable of discriminating the direction and magnitude of stimulations without further signal processing. Our tactile sensor is based on a flexible core and four sidewall structures of elastomer, where highly sensitive interlocking piezoresistive type sensing elements are embedded. We demonstrate the discriminating normal pressure and shear force simultaneously without interference between the applied forces. The developed sensor can detect down to 128 Pa in normal pressure and 0.08 N in shear force, respectively. The developed sensor can be applied in the prosthetic arms requiring the restoration of tactile sensation to discriminate the feeling of normal and shear force like human skin.

Human-Inspired Tactile Perception System for Real-Time and Multimodal Detection of Tactile Stimuli.

A human can intuitively perceive and comprehend complicated tactile information because the cutaneous receptors distributed in the fingertip skin receive different tactile stimuli simultaneously and the tactile signals are immediately transmitted to the brain. Although many research groups have attempted to mimic the structure and function of human skin, it remains a challenge to implement human-like tactile perception process inside one system. In this study, we developed a real-time and multimodal tactile system that mimics the function of cutaneous receptors and the transduction of tactile stimuli from receptors to the brain, by using multiple sensors, a signal processing and transmission circuit module, and a signal analysis module. The proposed system is capable of simultaneously acquiring four types of decoupled tactile information with a compact system, thereby enabling differentiation between various tactile stimuli, texture characteristics, and consecutive complex motions. This skin-like three-dimensional integrated design provides further opportunities in multimodal tactile sensing systems.

Low-Voltage Stretchable Electroluminescent Loudspeakers with Synchronous Sound and Light Generation.

Stretchable sound-in-displays, which can generate synchronous sound and light directly from the display without a separate speaker, allow immersive audio and visual perception even on curved surfaces. In stretchable sound-in-displays, alternating current electroluminescent (ACEL) devices have been used as light-emitting sources owing to their high brightness and stability. However, stretchable ACEL devices that use low dielectric constant (κ) materials require a high operating voltage for generating light and sound. Herein, we demonstrate a stretchable ACEL loudspeaker with a low operating voltage using stretchable high-κ dielectrics and strain-insensitive electrodes. Our device exhibits 87.7 cd/m2 of luminance and 79.70 dB of sound pressure level at an operating voltage of 120 V and 10 kHz. As the next platform of wearable devices, the suggested ACEL loudspeaker exhibits high-quality synchronous light and sound generation performance even under various types of mechanical deformation, such as finger flexion and wrist bending.

Femtosecond-resolved imaging of a single-particle phase transition in energy-filtered ultrafast electron microscopy.

Using an energy filter in transmission electron microscopy has enabled elemental mapping at the atomic scale and improved the precision of structural determination by gating inelastic and elastic imaging electrons, respectively. Here, we use an energy filter in ultrafast electron microscopy to enhance the temporal resolution toward the domain of atomic motion. Visualizing transient structures with femtosecond temporal precision was achieved by selecting imaging electrons in a narrow energy distribution from dense chirped photoelectron packets with broad longitudinal momentum distributions and thus typically exhibiting picosecond durations. In this study, the heterogeneous ultrafast phase transitions of vanadium dioxide (VO2) nanoparticles, a representative strongly correlated system, were filmed and attributed to the emergence of a transient, low-symmetry metallic phase caused by different local strains. Our approach enables electron microscopy to access the time scale of elementary nuclear motion to visualize the onset of the structural dynamics of matter at the nanoscale.

Multi-Layered Triboelectric Nanogenerators with Controllable Multiple Spikes for Low-Power Artificial Synaptic Devices.

In the domains of wearable electronics, robotics, and the Internet of Things, there is a demand for devices with low power consumption and the capability of multiplex sensing, memory, and learning. Triboelectric nanogenerators (TENGs) offer remarkable versatility in this regard, particularly when integrated with synaptic transistors that mimic biological synapses. However, conventional TENGs, generating only two spikes per cycle, have limitations when used in synaptic devices requiring repetitive high-frequency gating signals to perform various synaptic plasticity functions. Herein, a multi-layered micropatterned TENG (M-TENG) consisting of a polydimethylsiloxane (PDMS) film and a composite film that includes 1H,1H,2H,2H-perfluorooctyltrichlorosilane/BaTiO3 /PDMS are proposed. The M-TENG generates multiple spikes from a single touch by utilizing separate triboelectric charges at the multiple friction layers, along with a contact/separation delay achieved by distinct spacers between layers. This configuration allows the maximum triboelectric output charge of M-TENG to reach up to 7.52 nC, compared to 3.69 nC for a single-layered TENG. Furthermore, by integrating M-TENGs with an organic electrochemical transistor, the spike number multiplication property of M-TENGs is leveraged to demonstrate an artificial synaptic device with low energy consumption. As a proof-of-concept application, a robotic hand is operated through continuous memory training under repeated stimulations, successfully emulating long-term plasticity.

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.

Shape-Configurable MXene-Based Thermoacoustic Loudspeakers with Tunable Sound Directivity.

Film-type shape-configurable speakers with tunable sound directivity are in high demand for wearable electronics. Flexible, thin thermoacoustic (TA) loudspeakers-which are free from bulky vibrating diaphragms-show promise in this regard. However, configuring thin TA loudspeakers into arbitrary shapes is challenging because of their low sound pressure level (SPL) under mechanical deformations and low conformability to other surfaces. By carefully controlling the heat capacity per unit area and thermal effusivity of an MXene conductor and substrates, respectively, it fabricates an ultrathin MXene-based TA loudspeaker exhibiting high SPL output (74.5 dB at 15 kHz) and stable sound performance for 14 days. Loudspeakers with the parylene substrate, whose thickness is less than the thermal penetration depth, generated bidirectional and deformation-independent sound in bent, twisted, cylindrical, and stretched-kirigami configurations. Furthermore, it constructs parabolic and spherical versions of ultrathin, large-area (20 cm × 20 cm) MXene-based TA loudspeakers, which display sound-focusing and 3D omnidirectional-sound-generating attributes, respectively.

Multifunctional, flexible electronic systems based on engineered nanostructured materials.

The development of flexible electronic systems has been extensively researched in recent years, with the goal of expanding the potential scope and market of modern electronic devices in the areas of computation, communications, displays, sensing and energy. Uniquely, the use of soft polymeric substrates enables the incorporation of advanced features beyond mechanical bendability and stretchability. In this paper, we describe several functionalities which can be achieved using engineered nanostructured materials. In particular, reversible binding, self-cleaning, antireflective and shape-reconfigurable properties are introduced for the realization of multifunctional, flexible electronic devices. Examples of flexible systems capable of spatial mapping and/or responding to external stimuli are also presented as a new class of user-interactive devices.

Optically- and thermally-responsive programmable materials based on carbon nanotube-hydrogel polymer composites.

A simple approach is described to fabricate reversible, thermally- and optically responsive actuators utilizing composites of poly(N-isopropylacrylamide) (pNIPAM) loaded with single-walled carbon nanotubes. With nanotube loading at concentrations of 0.75 mg/mL, we demonstrate up to 5 times enhancement to the thermal response time of the nanotube-pNIPAM hydrogel actuators caused by the enhanced mass transport of water molecules. Additionally, we demonstrate the ability to obtain ultrafast near-infrared optical response in nanotube-pNIPAM hydrogels under laser excitation enabled by the strong absorption properties of nanotubes. The work opens the framework to design complex and programmable self-folding materials, such as cubes and flowers, with advanced built-in features, including tunable response time as determined by the nanotube loading.

Ultrasensitive Multimodal Tactile Sensors with Skin-Inspired Microstructures through Localized Ferroelectric Polarization.

Multifunctional electronic skins have attracted considerable attention for soft electronics including humanoid robots, wearable devices, and health monitoring systems. Simultaneous detection of multiple stimuli in a single self-powered device is desired to simplify artificial somatosensory systems. Here, inspired by the structure and function of human skin, an ultrasensitive self-powered multimodal sensor is demonstrated based on an interlocked ferroelectric copolymer microstructure. The triboelectric and pyroelectric effects of ferroelectric microstructures enable the simultaneous detection of mechanical and thermal stimuli in a spacer-free single device, overcoming the drawbacks of conventional devices, including complex fabrication, structural complexity, and high-power consumption. Furthermore, the interlocked microstructure induces electric field localization during ferroelectric polarization, leading to enhanced output performance. The multimodal tactile sensor provides ultrasensitive pressure and temperature detection capability (2.2 V kPa-1 , 0.27 nA °C-1 ) over a broad range (0.1-98 kPa, -20 °C < ΔT < 30 °C). Furthermore, multiple simultaneous stimuli can be distinguished based on different response times of triboelectric and pyroelectric effects. The remarkable performance of this sensor enables real-time monitoring of pulse pressure, acoustic wave detection, surface texture analysis, and profiling of multiple stimuli.

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.

Dynamic and Reprocessable Fluorinated Poly(hindered urea) Network Materials Containing Ionic Liquids to Enhance Triboelectric Performance.

Triboelectric nanogenerators (TENGs), a newly developed energy harvesting device that converts surrounding environmental mechanical stimuli into electricity, have been significantly explored as an ideal long-term power source for electrical devices. Despite recent advances, the development of advanced TENG devices with sufficient outputs to sustainably power electronic devices and rapid self-healability under mild conditions to improve their lifetime and function is highly demanded. Here, we report a robust self-healable and reprocessable TENG fabricated with a covalent adaptive network based on mechanically strong fluorinated poly(hindered urea) (F-PHU) integrated with ionic liquid as an efficient dielectric material to improve its triboelectric efficiency and self-healing capability simultaneously. The synthesis and integration of a well-defined reactive copolymer having both pendant fluorinated and t-butylamino bulky groups are the key to fabricate robust F-PHU networks containing fluorinated dangling chains that can interact with ionic liquids to induce ionic polarization, which raises the dielectric constant and thus increases triboelectric performance. They also are cross-linked with dynamic bulky urea linkages for rapid self-healability and high reprocessability through their reversible exchange reactions at moderate temperatures. The developed ionic F-PHU materials exhibit a high TENG output performance (power density of 173.0 mW/m2) as well as high TENG output recovery upon repairing their surface damages. This work demonstrates that such a synergistic design of triboelectric ionic F-PHU materials could have great potential for applications requiring high-performance and long-lasting energy harvesting.