Broadband nonlinear conversion and random quasi-phase-matching in transparent glass composite.

With the development of laser technology, nonlinear optics plays a crucial role in frequency conversion. However, the generation of second harmonics in nonlinear optical crystals is generally subject to rigorous phase-matching conditions that hinder the performance of broadband tunability. It is believed that introducing disorders in nonlinear optical materials is helpful to overcome this obstacle. In this work, we have prepared a nonlinear microcrystal-doped glass (NMG) composite material, allowing for tunable and polarization-independent nonlinear conversion from visible to near-infrared. The linear dependence of SHG intensity versus sample thickness indicated the facilitation of random quasi-phase matching by using the NMG. Our results provide a more stable and promising platform for disordered nonlinear photonic materials and suggest the possibility of more efficient nonlinear conversions using the NMG composite glass fibers in future.

Observing Proton-Electron Mixed Conductivity in Graphdiyne.

Mixed conducting materials with both ionic and electronic conductivities have gained prominence in emerging applications. However, exploring material with on-demand ionic and electronic conductivities remains challenging, primarily due to the lack of correlating macroscopic conductivity with atom-scale structure. Here, the correlation of proton-electron conductivity and atom-scale structure in graphdiyne is explored. Precisely adjusting the conjugated diynes and oxygenic functional groups in graphdiyne yields a tunable proton-electron conductivity on the order of 103. In addition, a wet-chemistry lithography technique for uniform preparation of graphdiyne on flexible substrates is provided. Utilizing the proton-electron conductivity and mechanical tolerance of graphdiyne, bimodal flexible devices serving as capacitive switches and resistive sensors are created. As a proof-of-concept, a breath-machine interface for sentence-based communication and self-nursing tasks with an accuracy of 98% is designed. This work represents an important step toward understanding the atom-scale structure-conductivity relationship and extending the applications of mixed conducting materials to assistive technology.

Multiscale Heterogeneities-Based Piezoresistive Interfaces with Ultralow Detection Limitation and Adaptively Switchable Pressure Detectability.

Mechanical compliance and electrical enhancement are crucial for pressure sensors to promote performances when perceiving external stimuli. Here we propose a bioinspired multiscale heterogeneity-based interface to adaptively regulate its structure layout and switch to desirable piezoresistive behaviors with ultralow detection limitation. In such a multiscale heterogeneities system, the micro-/nanoscale spiny Ag-MnO2 heterostructure contributes to an ultralow detection limitation of 0.008 Pa and can perceive minor pressure increments under preloads with high resolution (0.0083%). The macroscale heterogeneous orientation of the cellular backbone enables anisotropic deformation, allowing the sensor to switch to rational sensitivity and working range (e.g., 580 kPa-1 for 0-20 kPa/54 kPa-1 for 60-140 kPa) as required. The sensor's stepwise activation progresses from the micro-/nanoscale heterostructure to the macroscale heterogeneous orientation, which can adaptively match diverse sensing tasks in complex applications scenarios. This multiscale heterogeneous and switchable design holds immense potential in the development of intelligent electromechanical devices, including wearable sensors, soft robotics, and smart actuators.

Intrinsically elastic polymer ferroelectric by precise slight cross-linking.

Ferroelectrics are an integral component of the modern world and are of importance in electrics, electronics, and biomedicine. However, their usage in emerging wearable electronics is limited by inelastic deformation. We developed intrinsically elastic ferroelectrics by combining ferroelectric response and elastic resilience into one material by slight cross-linking of plastic ferroelectric polymers. The precise slight cross-linking can realize the complex balance between crystallinity and resilience. Thus, we obtained an elastic ferroelectric with a stable ferroelectric response under mechanical deformation up to 70% strain. This elastic ferroelectric exerts potentials in applications related to wearable electronics, such as elastic ferroelectric sensors, information storage, and energy transduction.

Enhancing Prosthetic Control through High-Fidelity Myoelectric Mapping with Molecular Anchoring Technology.

Myoelectric control utilizes electrical signals generated from the voluntary contraction of remaining muscles in an amputee's stump to operate a prosthesis. Precise and agile control requires low-level myoelectric signals (below 10% of maximum voluntary contraction, MVC) from weak muscle contractions such as phantom finger or wrist movements, but imbalanced calcium concentration in atrophic skin can distort the signals. This is due to poor ionic-electronic coupling between skin and electrode, which often causes excessive muscle contraction, fatigue, and discomfort during delicate tasks. To overcome this challenge, a new strategy called molecular anchoring is developed to drive hydrophobic molecular effectively interact with and embed into stratum corneum for high coupling regions between ionic fluxes and electronic currents. The use of hydrophobic poly(N-vinyl caprolactam) gel has resulted in an interface impedance of 20 kΩ, which is 1/100 of a commercial acrylic-based electrode, allowing the detection of ultralow myoelectric signals (≈1.5% MVC) that approach human limits. With this molecular anchoring technology, amputees operate a prosthesis with greater dexterity, as phantom finger and wrist movements are predicted with 97.6% accuracy. This strategy provides the potential for a comfortable human-machine interface when amputees accomplish day-to-day tasks through precise and dexterous myoelectric control.

Liquid Metal-Based Electronics for On-Skin Healthcare.

Wearable devices are receiving growing interest in modern technologies for realizing multiple on-skin purposes, including flexible display, flexible e-textiles, and, most importantly, flexible epidermal healthcare. A 'BEER' requirement, i.e., biocompatibility, electrical elasticity, and robustness, is first proposed here for all the on-skin healthcare electronics for epidermal applications. This requirement would guide the designing of the next-generation on-skin healthcare electronics. For conventional stretchable electronics, the rigid conductive materials, e.g., gold nanoparticles and silver nanofibers, would suffer from an easy-to-fail interface with elastic substrates due to a Young's modulus mismatch. Liquid metal (LM) with high conductivity and stretchability has emerged as a promising solution for robust stretchable epidermal electronics. In addition, the fundamental physical, chemical, and biocompatible properties of LM are illustrated. Furthermore, the fabrication strategies of LM are outlined for pure LM, LM composites, and LM circuits based on the surface tension control. Five dominant epidermal healthcare applications of LM are illustrated, including electrodes, interconnectors, mechanical sensors, thermal management, and biomedical and sustainable applications. Finally, the key challenges and perspectives of LM are identified for the future research vision.

Liquid Metal Based Nano-Composites for Printable Stretchable Electronics.

Liquid metal (LM) has attracted prominent attention for stretchable and elastic electronics applications due to its exceptional fluidity and conductivity at room temperature. Despite progress in this field, a great disparity remains between material fabrication and practical applications on account of the high surface tension and unavoidable oxidation of LM. Here, the composition and nanolization of liquid metal can be envisioned as effective solutions to the processibility-performance dilemma caused by high surface tension. This review aims to summarize the strategies for the fabrication, processing, and application of LM-based nano-composites. The intrinsic mechanism and superiority of the composition method will further extend the capabilities of printable ink. Recent applications of LM-based nano-composites in printing are also provided to guide the large-scale production of stretchable electronics.

Stable Long Cycling of Small Molecular Organic Acid Electrode Materials Enabled by Nonflammable Eutectic Electrolyte.

Small molecule organic acids as electrode materials possess the advantages of high theoretical capacity, low cost, and good processability. However, these electrode materials suffer from poor cycling stability due to the inevitable dissolution of organic molecules in the electrolytes. Here, a eutectic mixture of lithium bis(trifluoromethanesulfonyl)imide and N-methylamine is employed as a eutectic electrolyte in Li-ion batteries with small molecule organic acids as electrodes. To enhance the cycling stability of the electrolyte, fluoroethylene carbonate is used as an additive. The electrolyte exhibits nonflammability, high ionic conductivity, and good electrochemical stability. Molecular dynamics simulations and density functional theory are performed to further investigate the solvation chemistry of the eutectic electrolyte. The well-designed eutectic electrolyte inhibits the dissolution of terephthalic acid effectively and displays superior performance with a capacity retention of ≈84% after 2000 cycles at a high current density of 1 A g-1 . It also enables stable cycling of more than 900 cycles at a high current density of 2 A g-1 at 60 °C. This study provides a strategy to enhance the cycling stability and safety of Li-ion batteries with organic electrode materials.

Polymer Electrolytes as Energy-Harvesting Materials to Capture Electrical Energy from Dynamic Mechanical Deformations.

Ionic electroactive polymers (iEAPs) can generate electrical energy under bending deformations exhibiting great potential for fabricating energy harvesters from dynamic vibrating environments. According to a previous study, this flexoelectric energy-harvesting potential is explored in polymer electrolyte membrane (PEM) assemblies subjected to intermittent square wave bending modes. The above study reveals that the mechanoelectrical transduction is likely to be the consequence of ion polarization under a pressure gradient across the PEM thickness. To further evaluate the applicability of the PEM assemblies for harvesting energy from dynamic environments, oscillatory bending deformation is applied in the present study, whereby the complex flexoelectric coefficient corresponding to dynamic capacitance exhibits strong frequency dependence. At very high oscillatory bending frequencies, the ionic clouds inside the PEM assemblies cannot be fully polarized, and thus the corresponding energy output tends to become smaller. However, the PEM assemblies having higher ionic conductivities can enhance energy output at high frequencies. Of particular interest is that the incorporated ionic liquid (IL) is not only capable of effectively plasticizing the polymer network, but also expediting the ionic conductivity, thereby enhancing the electrical energy output, which in turn provides important design guidance for efficient polymer energy harvesters.

Study on the Crystallinity and Oxidation States of Nanoporous Anodized Tin Oxide Films Regulated by Annealing Treatment for Supercapacitor Application.

In this study, electrodeposition combined with anodization was employed to prepare a nanoporous tin oxide film on a pure copper substrate. It was found that annealing temperature played a critically significant role in regulating the crystallinity, pore size, and contents of different oxidation states of the anodized tin oxide film to affect the electrochemical performance. The study verified that SnOx films treated by optimized annealing at 500 °C with precisely controlling the nanoporous morphology and crystallinity displayed competitive specific capacitance at an appropriate ratio of Sn4+ to Sn2+. A maximum specific capacitance of 86.2 mF/cm2 could be achieved at this temperature, and the capacitance retention rate still exceeded 90% even after 8000 charge-discharge cycles. With properly designed annealing treatment, we implemented tin film anodization to obtain an optimized electrode with significantly enhanced electrochemical performance, which shows a promising application in the electrochemical field to prepare electrodes.

Bio-Inspired Multi-Mode Pain-Perceptual System (MMPPS) with Noxious Stimuli Warning, Damage Localization, and Enhanced Damage Protection.

The multi-mode pain-perceptual system (MMPPS) is essential for the human body to perceive noxious stimuli in all circumstances and make an appropriate reaction. Based on the central sensitization mechanism, the MMPPS can switch between different working modes and thus offers a smarter protection mechanism to human body. Accordingly, before injury MMPPS can offer warning of excessive pressure with normal pressure threshold. After injury, extra care on the periphery of damage will be activated by decreasing the pressure threshold. Furthermore, the MMPPS will gradually recover back to a normal state as damage heals. Although current devices can realize basic functions like damage localization and nociceptor signal imitating, the development of a human-like MMPPS is still a great challenge. Here, a bio-inspired MMPPS is developed for prosthetics protection, in which all working modes is realized and controlled by mimicking the central sensitization mechanism. Accordingly, the system warns one of a potential injury, identifies the damaged area, and subsequently offers extra care. The proposed system can open new avenues for designing next-generation prosthetics, especially make other smart sensing systems operate under complete protection against injuries.

Differentiation of Multiple Mechanical Stimuli by a Flexible Sensor Using a Dual-Interdigital-Electrode Layout for Bodily Kinesthetic Identification.

Human bodily kinesthetic sensing is generally complicated and ever-changing due to the diversity of body deformation as well as the complexity of mechanical stimulus, which is different from the unidirectional mechanical motion. So, there exists a huge challenge for current flexible sensors to accurately differentiate and identify what kind of external mechanical stimulus is exerted via analyzing digital signals. Here, we report a flexible dual-interdigital-electrode sensor (FDES) that consists of two interdigital electrodes and a highly pressure-sensitive porous conductive sponge. The FDES can precisely identify multiple mechanical stimuli, e.g., pressing, positive bending, negative bending, X-direction stretching, and Y-direction stretching, and convert them into corresponding current variation signals. Moreover, the FDES exhibits other exceptional properties, such as high sensitivity, stretchability, large measurement range, and outstanding stability, accompanied by simple structural design and low-cost processing simultaneously. Additionally, our FDES successfully identifies various complex activities of the human body, which lays a foundation for the further development of multimode flexible sensors.

All-Fabric Ultrathin Capacitive Sensor with High Pressure Sensitivity and Broad Detection Range for Electronic Skin.

Flexible pressure sensors have emerged as an indispensable part of wearable devices due to their application in physiological activity monitoring. To realize long-term on-body service, they are increasingly required for properties of conformability, air permeability, and durability. However, the enhancement of sensitivity remains a challenge for ultrathin capacitive sensors, particularly in the low-pressure region. Here, we introduced a highly sensitive and ultrathin capacitive pressure sensor based on a breathable all-fabric network with a micropatterned nanofiber dielectric layer, an all-fabric capacitive sensor (AFCS). This all-fabric network endows a series of exceptional performances, such as high sensitivity (8.31 kPa-1 under 1 kPa), ultralow detection limit (0.5 Pa), wide detection range (0.5 Pa to 80 kPa), and excellent robustness (10 000 dynamic cycles). Besides, the all-fabric structure provides other properties for the AFCS, e.g., high skin conformability, super thinness (dozens of micrometers), and exceptional air permeability. Our AFCS shows promising potential in breathing track, muscle activity detection, fingertip pressure monitoring, and spatial pressure distribution, paving way for comfortable skinlike epidermal electronics.

Flexoelectricity in Flexoionic Polymer Electrolyte Membranes: Effect of Thiosiloxane Modification on Poly(ethylene glycol) Diacrylate and Ionic Liquid Electrolyte Composites.

The present article entails the generation of flexoelectricity during cantilever bending of a solid polymer electrolyte membrane (PEM), composed of poly(ethylene glycol) diacrylate (PEGDA) precursor and ionic liquid (hexylmethylimidazolium hexafluorophosphate). The effects of thiosiloxane modification of PEGDA precursor on glass transition, ionic conductivity, and flexoelectric performance have been explored as a function of PEM composition. The glass transition temperature (Tg) of the PEM declines with increasing thiosiloxane amount in the PEGDA co-network, while the ionic conductivity improves. The PEM/compliant carbonaceous electrodes assemblies were assembled to determine the flexoelectric coefficients by monitoring electrical voltage/current outputs for various PEM compositions under the intermittent square-wave and dynamic oscillatory sine-wave deformation modes. Of particular interest is that the room temperature flexoelectric coefficient exhibits strong frequency dependence in the vicinity of 0.01-10 Hz, suggesting that ion polarization and ion transport through the ion-dipole complexed networks can still be affected by the mobile side chain branches even in the elastic regime of the covalently bonded PEGDA network. The in-depth understanding of the effect of thiosiloxane side chain on flexoelectricity generation is anticipated to have impact on the development of mechanoelectrical energy conversion devices for energy harvesting applications from natural and dynamical environment.

Poly(ethylene glycol) Diacrylate Based Electro-Active Ionic Elastomer.

Preparation and low voltage induced bending (converse flexoelectricity) of crosslinked poly(ethylene glycol) diacrylate (PEGDA), modified with thiosiloxane (TS) and ionic liquid (1-hexyl-3-methylimidazolium hexafluorophosphate) (IL) are reported. In between 2µm PEDOT:PSS electrodes at 1 V, it provides durable (95% retention under 5000 cycles) and relatively fast (2 s switching time) actuation with the second largest strain observed so far in ionic electro-active polymers (iEAPs). In between 40 nm gold electrodes under 8 V DC voltage, the film can be completely curled up (270° bending angle) with 6% strain that, to the best of the knowledge, is unpreceded among iEAPs. These results render great potential for the TS/PEGDA/IL based electro-active actuators for soft robotic applications.

Mechanoelectrical Transduction of Polymer Electrolyte Membranes: Effect of Branched Networks.

The role of side-chain branching in flexoelectric properties of a flexible, ionic solid polymer electrolyte membrane (PEM) has been investigated subjected to mechanical bending. These PEMs were synthesized via photopolymerization of the bifunctional poly(ethylene glycol) diacrylate (PEGDA) network attached with monofunctional poly(ethylene glycol) methyl ether acrylate (PEGMEA) branches in their ternary mixtures with lithium bis(tri-fluoromethane sulfonyl) imide (LiTFSI) salt. Both the PEGDA polymer precursor and PEGDMA side branches are capable of ionizing the lithium salt, but the dissociated lithium cations can also form the complexation with ether oxygen of PEGDA. With increasing PEGMEA content, not only the glass transition temperature is lowered, but also the ionic conductivity increases with temperature, which may be attributed to plasticization by dangling PEGMEA side chains. The flexoelectric responses of PEMs were investigated under various intermittent and oscillatory cantilever bending modes as a function of PEM composition and frequency. Last but not the least, the mechanoelectrical energy conversion was evaluated for various PEGDA/PEGMEA compositions and discussed its potential applications in energy harvesting from natural resources such as wind and wave motions.

Electroresponsive Ionic Liquid Crystal Elastomers.

This paper describes the preparation, physical properties, and electric bending actuation of a new class of active materials-ionic liquid crystal elastomers (iLCEs). It is demonstrated that iLCEs can be actuated by low-frequency AC or DC voltages of less than 1 V. The bending strains of the unoptimized first iLCEs are already comparable to the well-developed ionic electroactive polymers. Additionally, iLCEs exhibit several novel and superior features, such as the alignment that increases the performance of actuation, the possibility of preprogrammed actuation patterns at the level of the cross-linking process, and dual (thermal and electric) actuations in hybrid samples. Since liquid crystal elastomers are also sensitive to magnetic fields and can also be light sensitive, iLCEs have far-reaching potentials toward multiresponsive actuations that may have so far unmatched properties in soft robotics, sensing, and biomedical applications.