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.

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.

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.

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.

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.

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.

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.

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.

Ferroelectricity-Coupled 2D-MXene-Based Hierarchically Designed High-Performance Stretchable Triboelectric Nanogenerator.

Triboelectric nanogenerators based on the state-of-the-art functional materials and device engineering provide an exciting platform for future multifunctional electronics, but it remains challenging to realize due to the lack of in-depth understanding on the functional properties of nanomaterials that are compatible with microstructural engineering. In this study, a high-performance stretchable (∼60% strain) triboelectric nanogenerator is demonstrated via an interlocked microstructural device configuration sandwiched between silver-nanowire-(Ag-NW) electrodes and hierarchically engineered spongy thermoplastic polyurethane (TPU) polymer composite with ferroelectric barium-titanate-coupled (BTO-coupled) 2D MXene (Ti3C2Tx) nanosheets. The use of MXene results in an increase in the dielectric constant whereas the dielectric loss is lowered via coupling with the ferroelectricity of BTO, which increases the overall output performance of the nanogenerator. The spongy nature of the composite film increases the capacitance variation under deformation, which results in improved energy-conversion efficiency (∼79%) and pressure sensitivity (4.6 VkPa-1 and 2.5 mAkPa-1) of the device. With the quantum-mechanically calculated electronic structure, the device converts biomechanical energy to electrical energy and generates an open-circuit output voltage of 260 V, short-circuit output current of 160 mA/m2, and excellent power output of 6.65 W/m2, which is sufficient to operate several consumer electronics. Owing to its superior pressure sensitivity and efficiency, the device enables a broad range of applications including real-time clinical human vital-sign monitoring, acoustic sensing, and multidimensional gesture-sensing functionality of a robotic hand. Considering the ease of fabrication, excellent functionality of the hierarchical polymer nanocomposite, and outstanding energy-harvesting performance of nanogenerators, this work is expected to stimulate the development of next-generation self-powered technology.

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.

Frequency-selective acoustic and haptic smart skin for dual-mode dynamic/static human-machine interface.

Accurate transmission of biosignals without interference of surrounding noises is a key factor for the realization of human-machine interfaces (HMIs). We propose frequency-selective acoustic and haptic sensors for dual-mode HMIs based on triboelectric sensors with hierarchical macrodome/micropore/nanoparticle structure of ferroelectric composites. Our sensor shows a high sensitivity and linearity under a wide range of dynamic pressures and resonance frequency, which enables high acoustic frequency selectivity in a wide frequency range (145 to 9000 Hz), thus rendering noise-independent voice recognition possible. Our frequency-selective multichannel acoustic sensor array combined with an artificial neural network demonstrates over 95% accurate voice recognition for different frequency noises ranging from 100 to 8000 Hz. We demonstrate that our dual-mode sensor with linear response and frequency selectivity over a wide range of dynamic pressures facilitates the differentiation of surface texture and control of an avatar robot using both acoustic and mechanical inputs without interference from surrounding noise.

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.

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.

Spatiotemporal Measurement of Arterial Pulse Waves Enabled by Wearable Active-Matrix Pressure Sensor Arrays.

Wearable pressure sensors have demonstrated great potential in detecting pulse pressure waves on the skin for the noninvasive and continuous diagnosis of cardiac conditions. However, difficulties lie in positioning conventional single-point sensors on an invisible arterial line, thereby preventing the detection of adequate signal amplitude for accurate pulse wave analysis. Herein, we introduce the spatiotemporal measurements of arterial pulse waves using wearable active-matrix pressure sensors to obtain optimal pulse waveforms. We fabricate thin-film transistor (TFT) arrays with high yield and uniformity using inkjet printing where array sizes can be customizable and integrate them with highly sensitive piezoresistive sheets. We maximize the pressure sensitivity (16.8 kPa-1) and achieve low power consumption (101 nW) simultaneously by strategically modulating the TFT operation voltage. The sensor array creates a spatiotemporal pulse wave map on the wrist. The map presents the positional dependence of pulse amplitudes, which allows the positioning of the arterial line to accurately extract the augmentation index, a parameter for assessing arterial stiffness. The device overcomes the positional inaccuracy of conventional single-point sensors, and therefore, it can be used for medical applications such as arterial catheter injection or the diagnosis of cardiovascular disease in daily life.

Interdigitated Three-Dimensional Heterogeneous Nanocomposites for High-Performance Mechanochromic Smart Membranes.

Mechanochromic smart membranes capable of optical modulation have great potential in smart windows, artificial skins, and camouflage. However, the realization of high-contrast optical modulation based on light scattering activated at a low strain remains challenging. Here, we present a strategy for designing mechanochromic scattering membranes by introducing a Young's modulus mismatch between the two interdigitated polydimethylsiloxane phases with weak interfaces in a periodic three-dimensional (3D) structure. The refractive index-matched interfaces of the nanocomposite provide a high optical transparency of 93%. Experimental and computational studies reveal that the 3D heterogeneity facilitates the generation of numerous nanoscale debonds or "nanogaps" at the modulus-mismatching interfaces, enabling incident light scattering under tension. The heterogeneous scatterer delivers both a high transmittance contrast of >50% achieved at 15% strain and a maximum contrast of 82%. When used as a smart window, the membrane demonstrates effective diffusion of transmitting sunlight, leading to moderate indoor illumination by eliminating extremely bright or dark spots. At the other extreme, such a 3D heterogeneous design with strongly bonded interfaces can enhance the coloration sensitivity of mechanophore-dyed nanocomposites. This work presents insights into the design principles of advanced mechanochromic smart membranes.

A Fully Biodegradable Ferroelectric Skin Sensor from Edible Porcine Skin Gelatine.

High-performance biodegradable electronic devices are being investigated to address the global electronic waste problem. In this work, a fully biodegradable ferroelectric nanogenerator-driven skin sensor with ultrasensitive bimodal sensing capability based on edible porcine skin gelatine is demonstrated. The microstructure and molecular engineering of gelatine induces polarization confinement that gives rise the ferroelectric properties, resulting in a piezoelectric coefficient (d33) of ≈24 pC N-1 and pyroelectric coefficient of ≈13 µC m-2K-1, which are 6 and 11.8 times higher, respectively, than those of the conventional planar gelatine. The ferroelectric gelatine skin sensor has exceptionally high pressure sensitivity (≈41 mV Pa-1) and the lowest detection limit of pressure (≈0.005 Pa) and temperature (≈0.04 K) ever reported for ferroelectric sensors. In proof-of-concept tests, this device is able to sense the spatially resolved pressure, temperature, and surface texture of an unknown object, demonstrating potential for robotic skins and wearable electronics with zero waste footprint.

Electronic Textiles Based on Highly Conducting Poly(vinyl alcohol)/Carbon Nanotube/Silver Nanobelt Hybrid Fibers.

Highly stable conducting fibers have attracted significant attention in electronic textile (e-textile) applications. Here, we fabricate highly conducting poly(vinyl alcohol) (PVA) nanocomposite fibers with high thermal and chemical stability based on silver nanobelt (AgNB)/multiwalled carbon nanotube (MWCNT) hybrid materials as conducting fillers. At 20 vol % AgNB/MWCNT, the electrical conductivity of the fiber dramatically increased (∼533 times) from 3 up to 1600 S/cm after thermal treatment at 300 °C for 5 min. Moreover, PVA/AgNB/MWCNT fiber resists the harsh conditions of good solvents for PVA as well as high temperatures over the melting point of PVA, whereas pure PVA fiber is unstable in these environments. The significantly enhanced electrical conductivity and chemical stability can be realized through the post-thermal curing process, which is attributed to the coalescence between adjacent AgNBs and additional intensive cross-linking of PVA. These remarkable characteristics make our conducting fibers suitable for applications in e-textiles such as water leakage detectors and wearable heaters. In particular, heating behavior of e-textiles by Joule heating can accelerate the desorption of physically trapped moisture from the fiber surface, resulting in the fully reversible operation of water leakage monitoring. This smart e-textile sensor based on highly stable and conductive composite fibers will pave the way for diverse e-textile applications.

High-Performance Triboelectric Devices via Dielectric Polarization: A Review.

Energy harvesting devices based on the triboelectric effect have attracted great attention because of their higher output performance compared to other nanogenerators, which have been utilized in various wearable applications. Based on the working mechanism, the triboelectric performance is mainly proportional to the surface charge density of the triboelectric materials. Various approaches, such as modification of the surface functional group and dielectric composition of the triboelectric materials, have been employed to enhance the surface charge density, leading to improvements in triboelectric performances. Notably, tuning the dielectric properties of triboelectric materials can significantly increase the surface charge density because the surface charge is proportional to the relative permittivity of the triboelectric material. The relative dielectric constant is modified by dielectric polarization, such as electronic, vibrational (or atomic), orientation (or dipolar), ionic, and interfacial polarization. Therefore, such polarization represents a critical factor toward improving the dielectric constant and consequent triboelectric performance. In this review, we summarize the recent insights on the improvement of triboelectric performance via enhanced dielectric polarization.

Bioinspired Gradient Conductivity and Stiffness for Ultrasensitive Electronic Skins.

Hierarchical and gradient structures in biological systems with special mechanical properties have inspired innovations in materials design for construction and mechanical applications. Analogous to the control of stress transfer in gradient mechanical structures, the control of electron transfer in gradient electrical structures should enable the development of high-performance electronics. This paper demonstrates a high performance electronic skin (e-skin) via the simultaneous control of tactile stress transfer to an active sensing area and the corresponding electrical current through the gradient structures. The flexible e-skin sensor has extraordinarily high piezoresistive sensitivity at low power and linearity over a broad pressure range based on the conductivity-gradient multilayer on the stiffness-gradient interlocked microdome geometry. While stiffness-gradient interlocked microdome structures allow the efficient transfer and localization of applied stress to the sensing area, the multilayered structure with gradient conductivity enables the efficient regulation of piezoresistance in response to applied pressure by gradual activation of current pathways from outer to inner layers, resulting in a pressure sensitivity of 3.8 × 105 kPa-1 with linear response over a wide range of up to 100 kPa. In addition, the sensor indicated a rapid response time of 0.016 ms, a low minimum detectable pressure level of 0.025 Pa, a low operating voltage (100 µV), and high durability during 8000 repetitive cycles of pressure application (80 kPa). The high performance of the e-skin sensor enables acoustic wave detection, differentiation of gas characterized by different densities, subtle tactile manipulation of objects, and real-time monitoring of pulse pressure waveform.

Binary Spiky/Spherical Nanoparticle Films with Hierarchical Micro/Nanostructures for High-Performance Flexible Pressure Sensors.

Flexible pressure sensors have been widely explored for their versatile applications in electronic skins, wearable healthcare monitoring devices, and robotics. However, fabrication of sensors with characteristics such as high sensitivity, linearity, and simple fabrication process remains a challenge. Therefore, we propose herein a highly flexible and sensitive pressure sensor based on a conductive binary spiky/spherical nanoparticle film that can be fabricated by a simple spray-coating method. The sea-urchin-shaped spiky nanoparticles are based on the core-shell structures of spherical silica nanoparticles decorated with conductive polyaniline spiky shells. The simple spray coating of binary spiky/spherical nanoparticles enables the formation of uniform conductive nanoparticle-based films with hierarchical nano/microstructures. The two differently shaped particles-based films (namely sea-urchin-shaped and spherical) when interlocked face-to-face to form a bilayer structure can be used as a highly sensitive piezoresistive pressure sensor. Our optimized pressure sensor exhibits high sensitivity (17.5 kPa-1) and linear responsivity over a wide pressure range (0.008-120 kPa), owing to the effects of stress concentration and gradual deformation of the hierarchical microporous structures with sharp nanoscale tips. Moreover, the sensor exhibits high durability over 6000 repeated cycles and practical applicability in wearable devices that can be used for healthcare monitoring and subtle airflow detection (1 L/min).