Adaptive Gap-Tunable Surface-Enhanced Raman Spectroscopy.

Gap plasmon (GP) resonance in static surface-enhanced Raman spectroscopy (SERS) structures is generally too narrow and not tunable. Here, we present an adaptive gap-tunable SERS device to selectively enhance and modulate different vibrational modes via active flexible Au nanogaps, with adaptive optical control. The tunability of GP resonance is up to ∼1200 cm-1 by engineering gap width, facilitated by mechanical bending of a polyethylene terephthalate substrate. We confirm that the tuned GP resonance selectively enhances different Raman spectral regions of the molecules. Additionally, we dynamically control the SERS intensity through the wavefront shaping of excitation beams. Furthermore, we demonstrate simulation results, exhibiting the mechanical and optical properties of a one-dimensional flexible nanogap and their advantage in high-speed biomedical sensing. Our work provides a unique approach for observing and controlling the enhanced chemical responses with dynamic tunability.

Covalently-Bonded Laminar Assembly of Van der Waals Semiconductors with Polymers: Toward High-Performance Flexible Devices.

Van der Waals semiconductors (vdWS) offer superior mechanical and electrical properties and are promising for flexible microelectronics when combined with polymer substrates. However, the self-passivated vdWS surfaces and their weak adhesion to polymers tend to cause interfacial sliding and wrinkling, and thus, are still challenging the reliability of vdWS-based flexible devices. Here, an effective covalent vdWS-polymer lamination method with high stretch tolerance and excellent electronic performance is reported. Using molybdenum disulfide (MoS2 )and polydimethylsiloxane (PDMS) as a case study, gold-chalcogen bonding and mercapto silane bridges are leveraged. The resulting composite structures exhibit more uniform and stronger interfacial adhesion. This enhanced coupling also enables the observation of a theoretically predicted tension-induced band structure transition in MoS2 . Moreover, no obvious degradation in the devices' structural and electrical properties is identified after numerous mechanical cycle tests. This high-quality lamination enhances the reliability of vdWS-based flexible microelectronics, accelerating their practical applications in biomedical research and consumer electronics.

Gallium-Based Liquid Metals in Rechargeable Batteries: From Properties to Applications.

Gallium-based (Ga-based) liquid metals have attracted considerable interest due to their low melting points, enabling them to feature both liquid properties and metallic properties at room temperature. In light of this, Ga-based liquid metals also possess excellent deformability, high electrical and thermal conductivity, superior metal affinity, and unique self-limited surface oxide, making them popular functional materials in energy storage. This provides a possibility to construct high-performance rechargeable batteries that are deformable, free of dendrite growth, and so on. This review primarily starts with the property of Ga-based liquid metal, and then focuses on the potential applications in rechargeable batteries by exploiting these advantages, aiming to construct the correlation between properties and structures. The glorious applications contain interface protection, self-healing electrode construction, thermal management, and flexible batteries. Finally, the opportunities and obstacles for the applications of liquid metal in batteries are presented.

A 2.5 V In-Plane Flexi-Pseudocapacitor with Unprecedented Energy and Cycling Efficiency for All-Weather Applications.

As electronic devices for aviation, space, and satellite applications become more sophisticated, built-in energy storage devices also require a wider temperature spectrum. Herein, an all-climate operational, energy and power-dense, flexible, in-plane symmetric pseudocapacitor is demonstrated with utmost operational safety and long cycle life. The device is constructed with interdigital-patterned laser-scribed carbon-supported electrodeposited V5O12·6H2O as a binder-free electrode and a novel high-voltage anti-freezing water-in-salt-hybrid electrolyte. The anti-freezing electrolyte can operate over a wide temperature range of -40-60 °C while offering a stable potential window of ≈2.5 V. The device undergoes rigorous testing under diverse environmental conditions, including rapid and regular temperature and mechanical transition over multiple cycles. Additionally, detailed theoretical simulation studies are performed to understand the interfacial interactions with the active material as well as the local behavior of the anti-freeze electrolyte at different temperatures. As a result, the all-weather pseudocapacitor at 1 A g-1 shows a high areal capacitance of 234.7 mF cm-2 at room temperature and maintains a high capacitance of 129.8 mF cm-2 even at -40 °C. Besides, the cell operates very reliably for over 80 950 cycles with a capacitance of 25.7 mF cm-2 at 10 A g-1 and exhibits excellent flexibility and bendability under different stress conditions.

Flexible multifunctional titania nanotube array platform for biological interfacing.

Abstract: The current work presents a novel flexible multifunctional platform for biological interface applications. The use of titania nanotube arrays (TNAs) as a multifunctional material is explored for soft-tissue interface applications. In vitro biocompatibility of TNAs to brain-derived cells was first examined by culturing microglia cells-the resident immune cells of the central nervous system on the surface of TNAs. The release profile of an anti-inflammatory drug, dexamethasone from TNAs-on-polyimide substrates, was then evaluated under different bending modes. Flexible TNAs-on-polyimide sustained a linear release of anti-inflammatory dexamethasone up to ~11 days under different bending conditions. Finally, microfabrication processes for patterning and transferring TNA microsegments were developed to facilitate structural stability during device flexing and to expand the set of compatible polymer substrates. The techniques developed in this study can be applied to integrate TNAs or other similar nanoporous inorganic films onto various polymer substrates. Impact statement: Titania nanotube arrays (TNAs) are highly tunable and biocompatible structures that lend themselves to multifunctional implementation in implanted devices. A particularly important aspect of titania nanotubes is their ability to serve as nano-reservoirs for drugs or other therapeutic agents that slowly release after implantation. To date, TNAs have been used to promote integration with rigid, dense tissues for dental and orthopedic applications. This work aims to expand the implant applications that can benefit from TNAs by integrating them onto soft polymer substrates, thereby promoting compatibility with soft tissues. The successful direct growth and integration of TNAs on polymer substrates mark a critical step toward developing mechanically compliant implantable systems with drug delivery from nanostructured inorganic functional materials. Diffusion-driven release kinetics and the high drug-loading efficiency of TNAs offer tremendous potential for sustained drug delivery for scientific investigations, to treat injury and disease, and to promote device integration with biological tissues. This work opens new opportunities for developing novel and more effective implanted devices that can significantly improve patient outcomes and quality of life. Supplementary information: The online version contains supplementary material available at 10.1557/s43577-023-00628-y.

Stretchable and Skin-Mountable Temperature Sensor Array Using Reduction-Controlled Graphene Oxide for Dermatological Thermography.

Since thermometry of human skin is critical information that provides important aspects of human health and physiology, accurate and continuous temperature measurement is required for the observation of physical abnormalities. However, conventional thermometers are uncomfortable because of their bulky and heavy features. In this work, we fabricated a thin, stretchable array-type temperature sensor using graphene-based materials. Furthermore, we controlled the degree of graphene oxide reduction and enhanced the temperature sensitivity. The sensor exhibited an excellent sensitivity of 2.085% °C-1. The overall device was designed in a wavy meander shape to provide stretchability for the device so that precise detection of skin temperature could be performed. Furthermore, polyimide film was coated to secure the chemical and mechanical stabilities of the device. The array-type sensor enabled spatial heat mapping with high resolution. Finally, we introduced some practical applications of skin temperature sensing, suggesting the possibility of skin thermography and healthcare monitoring.

An Ultrathin Flexible Programmable Spin Logic Device Based on Spin-Orbit Torque.

Flexible electronic devices have shown increasingly promising value facilitating our daily lives. However, flexible spintronic devices remain in their infancy. Here, this research demonstrates a type of nonvolatile, low power dissipation, and programmable flexible spin logic device, which is based on the spin-orbit torque in polyimide (PI)/Ta/Pt/Co/Pt heterostructures fabricated via capillary-assisted electrochemical delamination. The magnetization switching ratio is shown to be about 50% for the flexible device and does not change after 100 cycles of bending, indicating the device has stable performance. By designing the path of pulse current, five Boolean logic gates AND, NAND, NOT, NOR, and OR can be realized in an integrated two-element device. Moreover, such peeling-off devices can be successfully transferred to almost any substrate, such as paper and human skin, and maintain high performance. The flexible PI/Ta/Pt/Co/Pt spin logic device serves as logic-in-memory architecture and can be used in wearable electronics.

Single-crystalline GaN microdisk arrays grown on graphene for flexible micro-LED application.

We report the growth of single-crystalline GaN microdisk arrays on graphene and their application in flexible light-emitting diodes (LEDs). Graphene layers were directly grown onc-sapphire substrates using chemical vapor deposition and employed as substrates for GaN growth. Position-controlled GaN microdisks were laterally overgrown on the graphene layers with a micro-patterned SiO2mask using metal-organic vapor-phase epitaxy. The as-grown GaN microdisks exhibited excellent single crystallinity with a uniform in-plane orientation. Furthermore, we fabricated flexible micro-LEDs by achieving heteroepitaxial growth ofn-GaN, InxGa1-xN/GaN multiple quantum wells, andp-GaN layers on graphene-coated sapphire substrates. The GaN micro-LED arrays were successfully transferred onto bendable substrates and displayed strong blue light emission under room illumination, demonstrating their potential for integration into flexible optoelectronic devices.

Study of Pressure Distribution in Floor Tiles with Printed P(VDF:TrFE) Sensors for Smart Surface Applications.

Pressure sensors integrated in surfaces, such as the floor, can enable movement, event, and object detection with relatively little effort and without raising privacy concerns, such as video surveillance. Usually, this requires a distributed array of sensor pixels, whose design must be optimized according to the expected use case to reduce implementation costs while providing sufficient sensitivity. In this work, we present an unobtrusive smart floor concept based on floor tiles equipped with a printed piezoelectric sensor matrix. The sensor element adds less than 130 µm in thickness to the floor tile and offers a pressure sensitivity of 36 pC/N for a 1 cm2 pixel size. A floor model was established to simulate how the localized pressure excitation acting on the floor spreads into the sensor layer, where the error is only 1.5%. The model is valuable for optimizing the pixel density and arrangement for event and object detection while considering the smart floor implementation in buildings. Finally, a demonstration, including wireless connection to the computer, is presented, showing the viability of the tile to detect finger touch or movement of a metallic rod.

Large-area vertically aligned 2D MoS2layers on TEMPO-cellulose nanofibers for biodegradable transient gas sensors.

Crystallographically anisotropic two-dimensional (2D) molybdenum disulfide (MoS2) with vertically aligned (VA) layers is attractive for electrochemical sensing owing to its surface-enriched dangling bonds coupled with extremely large mechanical deformability. In this study, we explored VA-2D MoS2layers integrated on cellulose nanofibers (CNFs) for detecting various volatile organic compound gases. Sensor devices employing VA-2D MoS2/CNFs exhibited excellent sensitivities for the tested gases of ethanol, methanol, ammonia, and acetone; e.g. a high response rate up to 83.39% for 100 ppm ethanol, significantly outperforming previously reported sensors employing horizontally aligned 2D MoS2layers. Furthermore, VA-2D MoS2/CNFs were identified to be completely dissolvable in buffer solutions such as phosphate-buffered saline solution and baking soda buffer solution without releasing toxic chemicals. This unusual combination of high sensitivity and excellent biodegradability inherent to VA-2D MoS2/CNFs offers unprecedented opportunities for exploring mechanically reconfigurable sensor technologies with bio-compatible transient characteristics.

Wide-Range Humidity-Temperature Hybrid Flexible Sensor Based on Strontium Titanate and Poly 3,4 Ethylenedioxythiophene Polystyrene Sulfonate for Wearable 3D-Printed Mask Applications.

In this paper, we report a fast, linear wide-range hybrid flexible sensor based on a novel composite of strontium titanate (SrTiO3) and poly 3,4 ethylenedioxythiophene polystyrene sulfonate (PEDOT: PSS) as a sensing layer. Inter-digitate electrodes (IDEs) were printed for humidity monitoring (finger: 250 µm; spacing: 140 µm; length: 8 mm) whilst a meander-based pattern was printed for the temperature measurement (meander thickness: 180 µm; spacing: 400 µm) on each side of the PET substrate using silver ink. Moreover, active layers with different concentration ratios were coated on the electrodes using a spray coating technique. The as-developed sensor showed an excellent performance, with a humidity measurement range of (10-90% RH) and temperature measurement range of (25-90 °C) with a fast response (humidity: 5 s; temperature: 4.2 s) and recovery time (humidity: 8 s; temperature: 4.4 s). The reliability of the sensor during mechanical bending of up to 5.5 mm was validated with a reliable performance. The sensor was also used in real-world applications to measure human respiration. For this, a suggested sensor-based autonomous wireless node was included in a 3D-printed mask. The manufactured sensor was an excellent contender for wearable and environmental applications because of its exceptional performance, which allowed for the simultaneous measurement of both quantities by a single sensing device.

Solar Seawater Distillation by Flexible and Fully Passive Multistage Membrane Distillation.

Solar-assisted distillation is considered promising to solve the freshwater supply for off-grid communities. In this work, a passive and flexible multistage membrane distillation (F-MSMD) device is devised to produce freshwater via solar distillation with the latent heat of vapor condensation being recycled to enhance its energy efficiency. By designing a siphon effect, source water is continuously wicked into the evaporation layer and the concentrated brine flows out of the device before reaching saturation, which successfully solves the otherwise challenge of salt accumulation inside the device. To achieve such siphon flow, the recycled paper is prepared from spent copy paper and used as the evaporation layer for efficient water delivery owing to its large pore size and high hydrophilicity. An eight-stage F-MSMD device exhibits a stable clean water production rate at 3.61 kg m-2 h-1 in the newly designed siphon-flow mode. This work provides a green route for designing a solar-assisted distillation device.

Polydopamine nanofilms for high-performance paper-based electrochemical devices.

Since the discovery of polydopamine (PDA), there has been a lot of progress on using this substance to functionalize many different surfaces. However, little attention has been given to prepare functionalized surfaces for the preparation of flexible electrochemical paper-based devices. After fabricating the electrodes on paper substrates, we formed PDA on the surface of the working electrode using a chemical polymerization route. PDA nanofilms on carbon were characterized by contact angle (CA) experiments, X-ray photoelectron spectroscopy, scanning electron microscopy, atomic force microscopy (topography and electrical measurements) and electrochemical techniques. We observed that PDA introduces chemical functionalities (RNH2 and RC═O) that decrease the CA of the electrode. Moreover, PDA nanofilms did not block the heterogeneous electron transfer. In fact, we observed one of the highest standard heterogeneous rate constants (ks ) for electrochemical paper-based electrodes (2.5 ± 0.1) × 10-3  cm s-1 , which is an essential parameter to obtain larger currents. In addition, our results suggest that carbonyl functionalities are ascribed for the redox activity of the nanofilms. As a proof-of-concept, the electrooxidation of nicotinamide adenine dinucleotide showed remarkable features, such as, lower oxidation potential, electrocatalytic peak currents more than 30 times higher when compared to unmodified paper-based electrodes and electrocatalytic rate constant (kobs ) of (8.2 ± 0.6) × 102  L mol-1  s-1 .

Layer exchange synthesis of multilayer graphene.

Low-temperature synthesis of multilayer graphene (MLG) on arbitrary substrates is the key to incorporating MLG-based functional thin films, including transparent electrodes, low-resistance wiring, heat spreaders, and battery anodes in advanced electronic devices. This paper reviews the synthesis of MLG via the layer exchange (LE) phenomenon between carbon and metal from its mechanism to the possibility of device applications. The mechanism of LE is completely different from that of conventional MLG precipitation methods using metals, and the resulting MLG exhibits unique features. Modulation of metal species and growth conditions enables synthesis of high-quality MLG over a wide range of growth temperatures (350 °C-1000 °C) and MLG thicknesses (5-500 nm). Device applications are discussed based on the high electrical conductivity (2700 S cm-1) of MLG and anode operation in Li-ion batteries. Finally, we discuss the future challenges of LE for MLG and its application to flexible devices.

Giant Wrinkles on the Surface of Epitaxial BaTiO3 Thin Films with Drastic Shrinkage during Transfer from a MgO(100) Single-Crystal Substrate to a Flexible Polyethylene Terephthalate Sheet.

The transfer of ferroelectric and piezoelectric BaTiO3 epitaxial thin films from an original MgO(100) single-crystal substrate to a polyethylene terephthalate (PET) sheet has been studied to fabricate flexible epitaxial functional oxides. The outline of our previous transfer process is as follows: the epitaxial BaTiO3 thin films were deposited on the MgO(100). Then, the surface of the BaTiO3 was adhered onto a PET sheet. Finally, only the MgO(100) substrate was dissolved in a phosphoric aqueous solution, which resulted in the transfer of the epitaxial BaTiO3 thin film from the MgO(100) to a PET sheet. To establish this transfer process, our aim was to prevent any damage, such as cracks and exfoliation, during the transfer of the epitaxial functional oxides. We found that a Pt buffer layer with a ductile nature was effective for improving the quality of transferred epitaxial BaTiO3 thin films. Moreover, the epitaxial BaTiO3 thin films showed a drastic shrinkage of ca. 10%. The surfaces of the shrunk, epitaxial BaTiO3 thin films showed giant wrinkles with a micrometer-order amplitude and a 10-µm-order periodicity without any damage. The epitaxial BaTiO3 thin films with giant wrinkles, accompanied by drastic shrinkage, are similar to the thin films that are coated on a pre-stretched elastomer, which is one of the fabrication processes of stretchable devices.

Nano-copper enhanced flexible device for simultaneous measurement of human respiratory and electro-cardiac activities.

BACKGROUND: Dysfunction of human respiratory and electro-cardiac activities could affect the ability of the heart to pump blood and the lungs to inhale oxygen. Thus, a device could simultaneously measure electro-cardiac signal and respiratory pressure could provide vital signs for predicting early warning of cardio-pulmonary function-related chronic diseases such as cardiovascular disease, and respiratory system disease. RESULTS: In this study, a flexible device integrated with piezo-resistive sensing element and voltage-sensing element was developed to simultaneously measure human respiration and electro-cardiac signal (including respiratory pressure, respiration frequency, and respiration rhythm; electro-cardio frequency, electro-cardio amplitude, and electro-cardio rhythm). When applied to the measurement of respiratory pressure, the piezo-resistive performance of the device was enhanced by nano-copper modification, which detection limitation of pressure can reduce to 100 Pa and the sensitivity of pressure can achieve to 0.053 ± 0.00079 kPa-1. In addition, the signal-to-noise ratio during bio-electrical measurement was increased to 10.7 ± 1.4, five times better than that of the non-modified device. CONCLUSION: This paper presents a flexible device for the simultaneous detection of human respiration and cardiac electrical activity. To avoid interference between the two signals, the layout of the electrode and the strain sensor was optimized by FEA simulation analysis. To improve the piezo-resistive sensitivity and bio-electric capturing capability of the device, a feather-shaped nano-copper was modified onto the surface of carbon fiber. The operation simplicity, compact size, and portability of the device open up new possibilities for multi-parameter monitoring.

A Flexible Film Bulk Acoustic Resonator Based on -Phase Polyvinylidene Fluoride Polymer.

This paper reports a novel flexible film bulk acoustic resonator (FBAR) based on -phase polyvinylidene fluoride (PVDF) piezoelectric polymer. The proposed device was simulated and evaluated; then, a low-temperature photolithography process with a double exposure method was developed to pattern the electrodes for the device, which enabled the device to retain the piezoelectric properties of the -phase PVDF film. Results showed that the ß-phase PVDF FBARs had a resonant frequency round 9.212 with a high electromechanical coupling coefficient () of 12.76% ± 0.56%. The device performed well over a wide bending-strain range up to 2400 owing to its excellent flexibility. It showed good stability as a strain sensor with a sensitivity of 80 , and no visible deterioration was observed after cyclic bending tests. The PVDF FBAR also exhibited an exceptionally large temperature coefficient of frequency (TCF) of -4630 , two orders of magnitude larger than those of other FBARs based on common inorganic piezoelectric materials, extraordinarily high sensitivity for temperature sensing. All results showed that -phase PVDF FBARs have the potential to expand the application scope for future flexible electronics.

Textile Based Electrochromic Cells Prepared with PEDOT: PSS and Gelled Electrolyte.

Electrochromic devices can act as passive displays. They change their color when a low voltage is applied. Flexible and bendable hybrid textile-film electrochromic devices with poly-3,4-ethylenedioxythiophene polystyrene sulfonate (PEDOT:PSS) were prepared on polyethylene polyethylene terephthalate (PEPES) membranes using a spray coating technique. The electrolyte consisted of a gelatin glycerol mixture as host matrix and calcium chloride. Titanium dioxide was used as an ion storage layer and a carbon containing dispersion was used for the counter electrode on a polyester rip-stop fabric. The sheet resistance of PEDOT:PSS on PEPES was 500 Ohm/sq. A 5 × 5 electrochromic matrix with individually addressable pixels was successfully designed and assembled. The switching time of the pixels was 2 s at a voltage of 2.0 V directly after assembling. The use of titanium dioxide as ion storage also increased the contrast of the dark-blue reduced electrochromic layer. Coloration was not self-sustaining. The PEDOT:PSS layer needed a constant low voltage of at least 0.5 V to sustain in the dark-blue reduced state. The switching time increased with time. After 12 months the switching time was ~4 s at a voltage of 2.8 V. The addition of glycerol into the electrolyte extended the lifetime of a non-encapsulated textile electrochromic cell, because moisture is retained in the electrolyte. Charge carriers can be transported into and out of the electrochromic layer.

Demonstration of Solar Cell on a Graphite Sheet with Carbon Diffusion Barrier Evaluation.

An amorphous Si (a-Si) solar cell with a back reflector composed of zinc oxide (ZnO) and silver (Ag) is potentially the most plausible and flexible solar cell if a graphite sheet is used as the substrate. Graphite supplies lightness, conductivity and flexibility to devices. When a graphite sheet is used as the substrate, carbon can diffuse into the Ag layer in the subsequent p-i-n process at 200-400 °C. To prevent this, we added an oxide layer as a carbon diffusion barrier between the carbon substrate and the back reflector. For the carbon diffusion barrier, silicon oxide (SiO2) or tin oxide (SnOx) was used. We evaluated the thermal stability of the back reflector of a carbon substrate using secondary-ion mass spectrometry (SIMS) to analyze the carbon diffusion barrier material. We confirmed the deposition characteristics, reflectance and prevention of carbon diffusion with and without the barrier. Finally, the structures were incorporated into the solar cell and their performances compared. The results showed that the back reflectors that were connected to a carbon diffusion barrier presented better performance, and the reflector with an SnOx layer presented the best performance.

A Self-Healing Metal-Organic Hydrogel for an All-Solid Flexible Supercapacitor.

A zinc containing metal-organic gel (Zn-MOG) with embedded free ions, which exhibits self-healing properties, has been synthesized for application in supercapacitors. The activated carbon-based flexible supercapacitor device with the MOG electrolyte has a broad potential window of 2.1 V, with high retention of specific capacitance compared to the traditional polyvinyl alcohol (PVA)-based gel. The Zn-MOG does not require an additional electrolyte. The sodium and sulphate ions embedded in the MOG are sufficient enough for the charge storage.