High-performance Flexible Devices Research Articles

Enhancing the performance of hydrogel strain/pressure sensors via gradient-entanglement-induced surface wrinkling patterns

Due to the advantages of high mechanical compliance and good biocompatibility, conductive hydrogels exhibit great application potential in flexible electronics. As the requirements in high sensitivity and high mechanical performance are increasing, the construction of patterned surfaces has been proven an effective approach, yet most of the common methods are complex and high-cost. Herein, we proposed a facile strategy to construct gradient entanglement dual network (GEDN) hydrogel with spontaneously patterned surface and consequent high surface area, which greatly enhances the sensitivity of hydrogel sensors. The strategy of high entanglement as well as the dual network in hydrogel achieved greatly improved mechanical performance. The prepared polyvinyl alcohol (PVA)/gradient entangled polyacrylamide (PAAm) DN and surface-patterned hydrogel possesses the advantages of excellent stretchability (681 %), high tensile strength (1.01 MPa), toughness (4.23 MJ/m3), and relatively low mechanical hysteresis. Meanwhile, it showed high sensitivity, wide detection range, and rapid response both as strain sensor (GFmax = 10.96, detection range = 681 %, an average response time of 170 ms) and pressure sensor (Smax = 0.17 kPa−1, detection range = 225 kPa, an average response time of 230 ms). In summary, it provides a new strategy for design of the multifunctional high-performance flexible devices, exhibiting great application prospects.

Crossmodal sensory neurons based on high-performance flexible memristors for human-machine in-sensor computing system

Constructing crossmodal in-sensor processing system based on high-performance flexible devices is of great significance for the development of wearable human-machine interfaces. A bio-inspired crossmodal in-sensor computing system can perform real-time energy-efficient processing of multimodal signals, alleviating data conversion and transmission between different modules in conventional chips. Here, we report a bio-inspired crossmodal spiking sensory neuron (CSSN) based on a flexible VO2 memristor, and demonstrate a crossmodal in-sensor encoding and computing system for wearable human-machine interfaces. We demonstrate excellent performance in the VO2 memristor including endurance (>1012), uniformity (0.72% for cycle-to-cycle variations and 3.73% for device-to-device variations), speed (<30 ns), and flexibility (bendable to a curvature radius of 1 mm). A flexible hardware processing system is implemented based on the CSSN, which can directly perceive and encode pressure and temperature bimodal information into spikes, and then enables the real-time haptic-feedback for human-machine interaction. We successfully construct a crossmodal in-sensor spiking reservoir computing system via the CSSNs, which can achieve dynamic objects identification with a high accuracy of 98.1% and real-time signal feedback. This work provides a feasible approach for constructing flexible bio-inspired crossmodal in-sensor computing systems for wearable human-machine interfaces.

Piezoelectric Enhancement in P(VDF-TrFE) Copolymer Films via Controlled and Template-Induced Epitaxy.

The surge in wearable electronics and Internet of Things technologies necessitates the development of both flexible sensors and a sustainable, efficient, and compact power source. The latter further challenges conventional batteries due to environmental pollution and compatibility issues. Addressing this gap, piezoelectric energy harvesters emerge as one kind of promising alternative to convert mechanical energy from ambient sources to electrical energy to charge those low-energy-consumption electronic devices. Despite slightly lower piezoelectric performance compared with those inorganic materials, piezoelectric polymers, notably poly(vinylidene fluoride-co-trifluoroethylene) P(VDF-TrFE), offer compelling properties for both flexible mechanical energy harvesting and self-powered strain/stress sensing, though their piezoelectric performance is expected to be further enhanced via varieties of modulation strategies of microstructures. Herein, we reported the controlled epitaxy process of micrometer-thick copolymer films with the cooperation of friction-transferred poly(tetrafluoroethylene) templates and precise modulation of the annealing conditions. Epitaxial P(VDF-TrFE) films present averaged d33 piezoelectric coefficient of -58.2 pC/N between 50 Hz and 1 kHz with good electromechanical and thermal stability. Owing to the nature of anisotropic crystallization, the epitaxial films exhibit an anisotropic transverse piezoelectric property. Epitaxial films were further utilized for mechanical energy harvesting and monitoring of human pulsation and respiration. This study provided a feasible route for the development of high-performance flexible piezoelectric devices to meet the requirement of flexible electronics.

Ductile P-Type AgCu(Se,S,Te) Thermoelectric Materials.

Ductile inorganic thermoelectric (TE) materials open a new approach to develop high-performance flexible TE devices. N-type Ag2(S,Se,Te) and p-type AgCu(Se,S,Te) pseudoternary solid solutions are two typical categories of ductile inorganic TE materials reported so far. Comparing with the Ag2(S,Se,Te) pseudoternary solid solutions, the phase composition, crystal structure, and physical properties of AgCu(Se,S,Te) pseudoternary solid solutions are more complex, but their relationships are still ambiguous now. In this work, via systematically investigating the phase composition, crystal structure, mechanical, and TE properties of about 60 AgCu(Se,S,Te) pseudoternary solid solutions, the comprehensive composition-structure-property phase diagrams of the AgCuSe-AgCuS-AgCuTe pseudoternary system is constructed. By mapping the complex phases, the "ductile-brittle" and "n-p" transition boundaries are determined and the composition ranges with high TE performance and inherent ductility are illustrated. On this basis, high performance p-type ductile TE materials are obtained, with a maximum zT of 0.81 at 340 K. Finally, flexible in-plane TE devices are prepared by using the AgCu(Se,S,Te)-based ductile TE materials, showing high output performance that is superior to those of organic and inorganic-organic hybrid flexible devices.

Damage-free dry transfer method using stress engineering for high-performance flexible two- and three-dimensional electronics.

Advanced transfer printing technologies have enabled the fabrication of high-performance flexible and stretchable devices, revolutionizing many research fields including soft electronics, optoelectronics, bioelectronics and energy devices. Despite previous innovations, challenges remain, such as safety concerns due to toxic chemicals, the expensive equipment, film damage during the transfer process and difficulty in high-temperature processing. Thus a new transfer printing process is needed for the commercialization of high-performance soft electronic devices. Here we propose a damage-free dry transfer printing strategy based on stress control of the deposited thin films. First, stress-controlled metal bilayer films are deposited using direct current magnetron sputtering. Subsequently, mechanical bending is applied to facilitate the release of the metal bilayer by increasing the overall stress. Experimental and simulation studies elucidate the stress evolution mechanisms during the processes. By using this method, we successfully transfer metal thin films and high-temperature-treated oxide thin films onto flexible or stretchable substrates, enabling the fabrication of two-dimensional flexible electronic devices and three-dimensional multifunctional devices.

Flexible visible and near-infrared laser detector based on bismuth sulphide nanorods

The development of a flexible, visible and near-infrared laser detector with fast response holds significant potential for applications in wearable electronics, binary switches, and other fields. In this study, we utilized a flexible transparent polyimide (PI) substrate known for its exceptional thermal resistance up to 400 °C to fabricate an innovative type of flexible laser detector. Systematic investigations demonstrate that the bismuth sulphide nanorods-based laser detector exhibits not only high flexibility and light-weight properties but also excellent linear current characteristics and strong photosensitive dependence on laser light intensity. This research presents a novel approach for the fabrication of high-performance flexible optoelectronic devices.

Highly Stable Silver Nanowire Plasmonic Electrodes for Flexible Polymer Light-Emitting Devices.

Silver nanowire (AgNW) transparent electrodes are considered as a promising candidate for applications in flexible optoelectronic devices. However, it remains a great challenge to obtain flexible AgNW electrodes with excellent optoelectrical properties and mechanical flexibility. Here, highly stable Ag nanoparticle (AgNP)-enhanced plasmonic AgNW electrodes are demonstrated via the controllable in situ growth of AgNPs at the AgNW junctions and introduction of an l-histidine (l-His) wrapping layer. The flexible transparent electrodes of AgNW-AgNP/l-His possess a low sheet resistance (Rsh) of ∼17.5 Ω sq-1, a high transmittance of ∼92.5% (550 nm), and a robust mechanical stability (100,000 bending cycles). Benefiting from plasmon-coupling effects, flexible polymer light-emitting devices (FPLEDs) with AgNW-AgNP/l-His electrodes present a current efficiency (CE) of ∼14.8 cd A-1 and an external quantum efficiency (EQE) of ∼5.6%, constituting ∼80% and ∼75% increases compared to those of the reference devices with AgNW electrodes, respectively. Additionally, the laminated flexible transparent PLEDs (FT-PLEDs) are demonstrated by integrating polydimethylsiloxane/AgNW-AgNP anodes by a soft lamination process. The FT-PLEDs present a CE of ∼7.1 cd A-1 (cathode side: ∼3.9 cd A-1; anode side: ∼3.2 cd A-1) and an EQE of ∼2.7% (cathode side: ∼1.5%; anode side: ∼1.2%). Furthermore, the FPLEDs and FT-PLEDs exhibit robust mechanical durability, maintaining ∼89% and ∼86% of their initial luminance after 1000 bending cycles at a bending radius of 2 mm, respectively. This work opens up a new avenue for the development of high performance and stable flexible optoelectronic devices.

High-performance flexible planner device featuring WS2 electrode and non-aqueous polymeric ionic electrolytes incorporated with ionic liquid and dual redox additives

Introducing redox-active species to enhance redox-activity at electrode–electrolyte interfaces, and designing the rational architecture of flexible supercapacitors comprising high-performance active materials and electrolytes with a wide potential window would be a key strategy to boost energy and power density. Herein, for the first time, we prepared an ionic liquid-based polymer electrolyte (IL/PE) by entrapping ionic liquid N-methyl-N-butyl pyrrolidinium bis (trifluoromethane sulfonyl) imide (P14TFSI)) in a polymer electrolyte Poly (diallyl dimethylammonium bis (trifluoromethane sulfonyl) imide (PDADMATFSI)) and blended with dual redox-additives (potassium iodide, KI and diphenylamine, DPA). The IL/PE with dual redox additives, demonstrates spectacular flexibility, high ionic conductivity (∼23.8 × 10−4 S cm−1), and stability in a wide potential window (∼5.9 V). A symmetrical interdigitated planner device is fabricated using dual redox-active IL/PE and flower-like WS2 electrode material. Benefiting from the synergistic effect of dual redox-active additive, the highest energy density of 47.86 µWh cm−2 at a power density of 3509 µW cm−2, and a high working potential (3 V) with excellent cycling stability upto 20,000 cycles has been achieved.

Compositionally engineered amorphous InZnO thin-film transistor with high mobility and stability via atmospheric pressure spatial atomic layer deposition

Amorphous indium-zinc oxide (IZO) thin films, featuring indium atomic concentrations between 35.2 and 64.2 at.%, were fabricated using atmospheric pressure spatial atomic layer deposition (AP S-ALD) at 250 °C, employing trimethylindium (TMI) and diethylzinc (DEZ) as precursors and ozone as the reactant, based on the atomic layer processing. The crystallinity and chemical bonding states of the IZO films were found to vary with the metal cation composition, as confirmed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). We fabricated thin-film transistors (TFTs) employing the IZO films as the active layer on polyimide (PI) substrates, achieving high mobility (45.7 cm2/V·s), excellent bias-temperature stress (BTS) stability (ΔVTH = 0.63 V), and maintaining stable electrical properties even after mechanical bending tests along two different axes. This study highlights the successful development of high-performance flexible devices by precisely controlling the metal cation composition using AP S-ALD based on high deposition rate.

Hummers' method-assisted liquid-phase exfoliation enables the fabrication of few-layer borophene from bulk boron.

The fabrication of few-layer borophene (BP) from bulk boron (b-B) is of great importance and still a scientific challenge due to the complex structure and crystallinity of b-B. Herein, we propose a novel technique to prepare a few-layer BP on a large scale with a large lateral size in a well-controlled manner. For this, we employed the Hummers' method-assisted liquid-phase exfoliation. In the first step, the chemical exfoliation of the b-B as a precursor was performed by the modified Hummers' method. After chemical exfoliation, mechanical delamination was employed by using an immersion sonicator. Finally, BP sheets were collected with dimensions ranging from several hundred nanometers to a few micrometers and an average thickness of 4.2 nm. We envision that the proposed low-cost, flexible, and large-scale production method will provide unique advantages for the application of few-layer BP in the realization of high-performance electronics, optoelectronics, flexible devices, sensing systems, energy conversion, and storage devices.

Metallic barrier layer for Ag2S1−xSex inorganic ductile thermoelectric materials

Metallic barrier layer is a key component in thermoelectric (TE) devices, but it is rarely investigated for the recently discovered inorganic ductile TE materials. In this work, we demonstrate that tungsten (W) is the excellent metallic barrier layer for Ag2S1−xSex ductile thermoelectric materials. The phase composition, microstructure, adhesive strength, and interfacial contact resistivity (ρC) of the W/Ag2S1−xSex joint have been systematically investigated. The sputtered W film has high adhesive strength and little interdiffusion/reaction with Ag2S1−xSex. The ρC decreases with increasing the Se content, which can be understood by the Thermionic-field Emission model. This work would guide the development of high-performance flexible TE devices based on ductile TE materials.

Synthesis, Characterization and Power Factor Estimation of SnSe Thin Film for Energy Harvesting Applications

In this work, a simple, cost-effective successive ionic layer adsorption and reaction (SILAR) deposition technique has been used to deposit a high-quality tin selenide (SnSe) thin film onto a glass substrate. Structural, morphologic, and thermoelectric properties have been characterized for the prepared thin film. X-ray diffraction (XRD) results of the SnSe thin film reveal an orthorhombic structure phase. The morphological properties of the prepared thin films have been studied using field emission scanning electron microscopy (FESEM). The stoichiometric composition of the deposited thin film and the elemental binding energies of the Sn and Se elements have been investigated with energy-dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). The Fourier transformation infrared (FTIR) spectrum of the SnSe thin film displays vibrational modes of chalcogenides bonds. These results suggest that the developed thin film is crystalline, uniform, and without impurities and is appropriate for energy harvesting applications. The prepared thin film’s Seebeck coefficient and electrical resistivity were estimated through ZEM-3 from room temperature to 600 K. The power factor was evaluated. A substantially high electrical conductivity is observed, which decreases somewhat with temperature, suggesting a semimetal conducting transport—the absolute values of the Seebeck coefficient increase with temperature. The resulting power factor showed the highest values near room temperature and a somewhat decreasing trend as the temperature increased. Despite lower values of the Seebeck coefficient, the substantially enhanced power factor is due to the higher electrical conductivity of the thin film, superior to that reported previously. This precursor study demonstrates promising results for developing high-performance flexible thermoelectric devices via a simple and facile SILAR strategy.

Enhanced polyvinyl alcohol ionic conductive hydrogel with feather keratin extracted via deep eutectic solvent for wearable strain sensor

The extraction of keratin from discarded feathers for the preparation of poly (vinyl alcohol) (PVA) ionic conductive hydrogels with enhanced mechanical properties shows promise for applications in green flexible electronics. Here, we first extracted feather keratin (FK) from duck feather fibers using the lactic acid/l-cysteine deep eutectic solvents. Subsequently, the composite ionic conductive hydrogel composed of FK, PVA, and CaCl2 was constructed by a one-pot freeze-thawing strategy. The introduction of FK resulted in a denser structure of the fabricated hydrogel, which significantly enhanced its mechanical properties, including high elongation at break of 639.3%, high breaking strength of 270 kPa, and durable fatigue resistance. Impressively, the hydrogel-based wearable strain sensor demonstrated high strain sensing sensitivity (GF = 1.26), wide strain detection range (5%–200%), fast response, and stable reliability, enabling it to accurately monitor and distinguish the difference in electrical signals generated by large and tiny human motions. This work provides a reliable method for the green extraction of FK and the design of high-performance PVA hydrogel-based flexible electrical devices.

Direct-Write Printed Slippery Surface for Assembling a High-Quality Graphene Structure and Its Application in Flexible Electric Actuators.

Graphene is a two-dimensional honeycomb-like nanomaterial generated by carbon atoms in sp2 hybridized orbitals to form a hexagonal lattice structure with excellent electrical, optical, and mechanical properties. The solution process method has been widely used to realize large-area patterned graphene structures for high-performance devices. In the method, graphene usually needs to be dispersed in solution, and the π-π bonding gravitational interactions between graphene sheets would lead to uncontrollable structures in solution and difficulty in obtaining high performance. In this work, a patterned graphene oxide (GO) structure with controllable thickness and layer spacing was realized by a direct-write printed slippery surface, which was used as a slippery limited template. After reducing GO into reduced graphene oxide (rGO), a flexible electric pattern with a conductivity of up to 6.425 × 103 S/m was realized. Furthermore, the patterned rGO structure was transferred on polydimethylsiloxane (PDMS), which could generate less than a 5% change in resistance after 10,000 consecutive bends, and an anisotropic expansion based on rGO and PDMS materials under electro-thermal coupling. The patterned rGO structures could meet the performance requirements of highly sensitive and complex deformation applications as flexible electric actuators. This study provides great research significance and application value for patterning high-quality graphene structures and realizing high-performance flexible electronic devices.

Ultrathin damage-tolerant flexible metal interconnects reinforced by in-situ graphene synthesis

Conductive patterned metal films bonded to compliant elastomeric substrates form meshes which enable flexible electronic interconnects for various applications. However, while bottom-up deposition of thin films by sputtering or growth is well-developed for rigid electronics, maintaining good electrical conductivity in sub-micron thin metal films upon large deformations or cyclic loading remains a significant challenge. Here, we propose a strategy to improve the electromechanical performance of nanometer-thin palladium films by in-situ synthesis of a conformal graphene coating using chemical vapor deposition (CVD). The uniform graphene coverage improves the thin film’s damage tolerance, electro-mechanical fatigue, and fracture toughness owing to the high stiffness of graphene and the conformal CVD-grown graphene-metal interface. Graphene-coated Pd thin film interconnects exhibit stable increase in electrical resistance even when strained beyond 60% and longer fatigue life up to a strain range of 20%. The effect of graphene is more significant for thinner films of < 300 nm, particularly at high strains. The experimental observations are well described by the thin film electro-fragmentation model and the Coffin-Manson relationship. These findings demonstrate the potential of CVD-grown graphene nanocomposite materials in improving the damage tolerance and electromechanical robustness of flexible electronics. The proposed approach offers opportunities for the development of reliable and high-performance ultra-conformable flexible electronic devices.

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.

Stable Flexible Electronic Devices under Harsh Conditions Enabled by Double-Network Hydrogels Containing Binary Cations.

Hydrogels are increasingly used in flexible electronic devices, but the mechanical and electrochemical stabilities of hydrogel devices are often limited under specific harsh conditions. Herein, chemically/physically cross-linked double-network (DN) hydrogels containing binary cations Zn2+ and Li+ are constructed in order to address the above challenges. Double networks of chemically cross-linked polyacrylamide (PAM) and physically cross-linked κ-Carrageenan (κ-CG) are designed to account for the mechanical robustness while binary cations endow the hydrogels with excellent ionic conductivity and outstanding environmental adaptability. Excellent mechanical robustness and ionic conductivity (25 °C, 2.26 S·m-1; -25 °C, 1.54 S·m-1) have been achieved. Utilizing the DN hydrogels containing binary cations as signal-converting materials, we fabricated flexible mechanosensors. High gauge factors (resistive strain sensors, 2.4; capacitive pressure sensors, 0.82 kPa-1) and highly stable sensing ability have been achieved. Interestingly, zinc-ion hybrid supercapacitors containing the DN hydrogels containing binary cations as electrolytes have achieved an initial capacity of 52.5 mAh·g-1 at a current density of 3 A·g-1 and a capacity retention rate of 82.9% after 19,000 cycles. Proper working of the zinc-ion hybrid supercapacitors at subzero conditions and stable charge-discharge for more than 19,000 cycles at -25 °C have been demonstrated. Overall, DN hydrogels containing binary cations have provided promising materials for high-performance flexible electronic devices under harsh conditions.

An Environment-Tolerant Ion-Conducting Double-Network Composite Hydrogel for High-Performance Flexible Electronic Devices

HighlightsNovel double-network (DN) ion-conducting hydrogel (ICH) based on a poly(ionic liquid)/MXene/poly(vinyl alcohol) system (named PMP DN ICH) was synthesized using freeze–thawing and ionizing radiation technology.The PMP DN ICH possesses a multiple cross-linking mechanism and exhibits outstanding ionic conductivity (63.89 mS cm−1), excellent temperature resistance (−60–80 °C) and decent mechanical performance.The well-designed PMP DN ICH shows considerable potential in wearable sensing, energy storage, and energy harvesting.

Low-temperature process design for inversion mode n-channel thin-film-transistor on polycrystalline Ge formed by solid-phase crystallization

We fabricated an inversion mode n-channel thin-film-transistor (TFT) on polycrystalline (poly-) Ge at low temperatures for monolithic three-dimensional large-scale IC (3D-LSI) and flexible electronics applications. Based on our previously reported solid-phase crystallization (SPC) method, we designed an n-channel TFT fabrication process with phosphorous ion implantation to provide the source/drain (S/D). We succeeded in fabricating an n-channel TFT with typical electrical characteristics on poly-Ge and confirmed its operation mode to be inversion mode. However, the fabrication process included a high temperature (500 °C) step for S/D activation. To reduce the process temperature, we used a metal-induced dopant activation method and successfully reduced the activation temperature to 360 °C. This combination is expected to pave the way for high-performance 3D-LSI and flexible electronic devices based on SPC-Ge.

Stability of Silver-Nanowire-Based Flexible Transparent Electrodes under Mechanical Stress

Flexible transparent electrodes are integral to the advancement of flexible optoelectronic devices such as flexible displays and solar cells. However, indium tin oxide (ITO), a traditional material used in transparent electrodes, exhibits a significant increase in resistance under mechanical stress, which limits the long-term stability of flexible devices. Here, we prepare various types of silver nanowire (AgNW)-based transparent electrodes and investigate their stability in terms of electrical resistance and optical transmittance under compressive and tensile stresses. Under compressive stress, ITO on a polyethylene terephthalate (PET) substrate exhibits a significantly high electrical resistance of &gt;3000 Ω after 1000 stress cycles, while the AgNW-coated electrode on a PET film exhibits a relatively smaller resistance of &lt;1200 Ω. The AgNW-embedded electrode in a UV-curable polymer matrix (NOA63 or NOA71) exhibits an even lower electrical resistance of &lt;450 Ω because AgNWs can easily maintain their network. A similar trend is observed under tensile stress. The AgNW-embedded electrode shows the highest resistance stability, whereas the ITO on the PET substrate shows the poorest stability. The optical transmittance is comparable regardless of the type of stress or electrode used. This superior stability of the AgNW-based electrodes, realized by integrating it with a polymer matrix, is promising for the development of durable and high-performance flexible optoelectronic devices.