Electroluminescent Devices Research Articles

Strain‐Insensitive Pre‐Stretch‐Stabilized Polymer/Gold Hybrid Electrodes for Electrochemiluminescent Devices

AbstractThe quest for stretchable properties is at the forefront of research dedicated to on‐skin light–emitting devices. Inspired by the natural wonders of bioluminescence, electrochemiluminescent devices (ECLDs) are distinguished by straightforward design and reduced operating voltage, marking a departure from traditional current‐driven electroluminescent devices (ACELDs). The primary challenge of fully‐stretchable ECLDs lies in crafting electrodes that simultaneously satisfy the demands for conductivity, transparency, stretchability, oxidation resistance, and interface stability. This research introduces a groundbreaking wrinkled polymer‐gold composite electrode. It extends to 50% stretchability, offers outstanding conductivity at 10 Ω sq−1, achieves transparency above 60%, and withstands over 10 000 stretching cycles. Employing this material, alongside stretchable electrospinning fiber luminescent layers, enabled the creation of fully‐stretchable ECLDs. These devices not only shine brightly at 30 Cd m−2 but also retain more than 90% of luminosity when stretched up to 50%. Furthermore, this work has engineered stretchable devices featuring singular patterns and multi‐dot arrays. They exhibit consistent luminescent output under bending, twisting, and stretching when applied to skin. These findings not only highlight the potential of polymer‐gold composite electrodes in overcoming challenges faced by stretchable electronic devices but also provide new ideas for wearable technology that seamlessly integrates with human body.

Shelf-Stable Green and Blue Quantum Dot Light-Emitting Diodes with High Efficiencies.

Quantum dot light-emitting diodes (QLEDs) are promising electroluminescent devices for next-generation display and solid-state lighting technologies. Achieving shelf-stable and high-performance QLEDs is crucial for their practical applications. However, the successful demonstration of shelf-stable QLEDs with high efficiencies is limited to red devices. Here, we developed a solution-based amine ligand exchange strategy to passivate the surfaces of optical ZnO (O-ZnO) nanocrystals, leading to suppressed exciton quenching at the green and blue QD/oxide interface. Furthermore, we designed new bilayered oxide electron-transporting layers consisting of amine-modified O-ZnO/conductive ZnO. This design simultaneously offers suppressed interfacial exciton quenching and sufficient electron transport in the green and blue QLEDs, resulting in shelf-stable green and blue devices with high efficiencies. Our devices exhibit neglectable changes in external quantum efficiencies (maximum external quantum efficiencies of 22.4% for green and 14.3% for blue) after storage for 270 days. Our work represents a step forward in the practical applications of QLED technology.

Tail-group tailoring for narrower green electroluminescence: The role of methoxysilane derivatives in QLEDs

Metal halide perovskite nanocrystals (PeNCs) are garnering significant interest as the future of light-emitting materials, primarily due to their exceptional emission characteristics, which include strong excitonic absorption and narrow-band, high-intensity emission. These properties are intricately linked to the surface chemistry of the nanocrystals, which can be effectively manipulated through the choice of ligands and specific reaction conditions during synthesis or subsequent ligand exchanges. In the first, we explore the ligand exchange processing in hexane with thiol-functionalized methoxysilanes, notable for their short chain and bifurcated structure. In the case of surface-modified PeNCs using methoxysilane, strain engineering is dominated by the tail group, which plays an even more important role than size dispersion in their effects on color purity and gamut. In addition, the methoxysilane ligand-induced lattice strain may also significantly alter charge transporting hehavior, as is demonstrated on zinc oxide (ZnO) using 3-aminopropyltrimethoxysilane (APTMS). These interesting observations arise from nanostrained optoelectronic materials, and are attractive for the development of high-purity electroluminescence devices.

Two novel bipolar materials based on 9,9-dimethylfluorene bridges for non-doped blue and red phosphorescent OLED applications

The present study delineates the design and synthesis of two bipolar host materials, namely 4-(7-(9-([1,1′-biphenyl]-4-yl)-9H-carbazol-3-yl)-9,9-dimethyl-9H-fluoren-2-yl)benzonitrile (o-CzDFBN) and 4-(7-(9-([1,1′-biphenyl]-3-yl)-9H-carbazol-3-yl)-9,9-dimethyl-9H-fluoren-2-yl)benzonitrile (p-CzDFBN). By incorporating 9,9-dimethylfluorene as a π conjugated bridge, the fluorescence quantum yield, carrier mobility and balance can be improved. Both host materials have excellent thermal stability, with thermal decomposition temperature (Td) of exceeding 390 °C and glass transition temperature (Tg) of exceeding 125 °C. Electroluminescent devices using p-CzDFBN as the host material show better performance than those based on o-CzDFBN. The maximum external quantum efficiencyof red PhOLED reaches 27.17%. The non-doped blue OLED achieves a EQEmax of 6.38%, a maximum luminance (Lmax) of 20150 cd/m2, a maximum current efficiency of 4.81 cd/A, and a maximum power efficiency of 5.40 lm/W. This research contributes to the development of new materials for OLEDs, potentially leading to more efficient, stable, and high-performing OLEDs.

Resilient, environment tolerant and biocompatible electroluminescent devices with enhanced luminance based on compliant and self-adhesive electrodes

Electroluminescent (EL) devices are of great significance for expanding the application range of optoelectronics. However, the realization of EL devices with environment-tolerance, stretchability, mechanical cycling stability, self-adhesion, biocompatibility, and high dielectric constant still remains a challenge. Herein, a type of EL device with enhanced comprehensive performances composing of a chlorinated barium titanate/phosphor/polydimethylsiloxane (Cl-BT/phosphor/PDMS) luminescent layer sandwiched between two silver nanowire-cellulose nanocrystal with II crystalline allomorph/Triton X-100 modified polydimethylsiloxane (AgNW-CNC II/TX-PDMS) electrodes fabricated through a full solution-processing strategy is proposed. Environmentally-friendly CNC II with high transmittance acts as an antioxidant, dispersant and film-former for AgNWs. The hydrophilic modification of TX to PDMS imparts the electrodes with self-adhesion, high stretchability, as well as strong interfacial bonding between TX-PDMS and AgNW-CNC II. The electrodes achieve skin-like modulus by adjusting TX content, endowing the EL devices with a high compliance (186 kPa of Young’s modulus). The luminescent layer with Cl-BT exhibits a high dielectric constant (19) and luminance (up to 72 cd m−2). The assembled EL device with excellent cyclic stability (luminance retention 85% after 400 cycles), durability (luminance retention >94% after 400 min) and stretchability (88% luminance at 200% strain) can work properly at broad temperatures (−20 ~ 70 °C) and underwater. This biocompatible and self-adhesive EL device demonstrates great potential for implantable biomedical devices and wearable displays under harsh environments.

Hot Exciton versus Hot Exciplex TADF Mechanism – Effect of the Donor‐Acceptor Functionalization Pattern on Anthracene‐based Emitters

Hot exciton emitters based on 9,10‐substituted anthracenes are a well‐investigated class of molecules featuring thermally activated delayed fluorescence (TADF). TADF converts triplet excitons into singlet excitons and improve the internal quantum efficiency of electroluminescent devices to performance beyond the limit of spin‐statistics of conventional emitters. In this paper, we compare different 1,8‐functionalized donor/acceptor‐substituted anthracenes and compare these to established 9,10‐functionalized hot exciton emitters. Interestingly, our new 1,8‐substituted anthracenes make use of a beneficial hot exciplex pathway, resulting in improved emission characteristics and higher photoluminescence quantum yield.

Elastomers based on polynorbornene with polar polysiloxane brushes for soft transducer applications

Elastomers based on cross‐linked bottlebrush polymers combine an extreme softness at low strains with a strain‐stiffening effect, which makes them attractive as active components in dielectric elastomer actuators (DEA). Their main disadvantage concerns the small relative permittivity, which lies in the range of 3.5, requiring relatively high driving voltage in actuators. We synthesized a bottlebrush polymeric elastomer with polar brushes, which exhibit an enhanced dielectric permittivity of 4.4. Anionic ring‐opening polymerization of a polar cyclosiloxane afforded telechelic polar brushes, while ring‐opening polymerization of a norbornene macromonomer gave a bottlebrush polymer which was cross‐linked to elastomers by a thiol‐ene reaction. Elastomers with a small elastic modulus below 100 kPa, strain at break exceeding 100%, attractive elasticity, and small mechanical loss factors (tanδ) were achieved. Temperature‐dependent impedance measurements revealed a transition temperature of ‐95 °C and an interfacial polarization. The multigram scale synthesis demonstrates the potential for scaling up, which opens the door to broader applications of these materials beyond actuators, such as capacitive sensors, batteries, and electroluminescent devices. Notably, these devices operate at extremely low voltages where the dielectric breakdown does not limit their functionality, but still, the softness and the increased dielectric permittivity are a plus.

Low Driving Voltage Electroluminescence Device for Integrated Visual Strain Sensing.

As a pivotal component in human-machine interactions, display devices have undergone rapid development in modern life. Displays such as alternative current electroluminescence|alternative current electroluminescent (ACEL) devices with high flexibility and long operational lifetimes are essential for wearable electronics. However, ACEL devices are constrained by their inherent high driving voltage and complex fabrication processes. Our work presents an easy blade-coating method for fabricating flexible ACEL display devices based on an all-solution process. By dispersing BaTiO3 and ZnS/Cu powder into waterborne polyurethane, we successfully combined dielectric and fluorescence functionalities within a single layer, significantly reducing the device's driving voltage. Additionally, the ionic conducting hydrogel was chosen as a transparent electrode to achieve good electrical contact and strong interfacial adhesion through in situ polymerization. Owing to the unique method, our ACEL device exhibits high flexibility, low driving voltage (20-100 V), high brightness (300+ cd/m2 at 60 V), and environmental friendliness. Furthermore, by repurposing the hydrogel electrode, we integrated strain visualization capabilities within a single device, highlighting its potential for applications such as wearable healthcare monitoring.

Multicolour stretchable perovskite electroluminescent devices for user-interactive displays

Wearable displays require mechanical deformability to conform to the skin, as well as long-term stability, multicolour emission and sufficient brightness to enable practically useful applications. However, endowing a single device with all the features remains a challenge. Here we present a rational material design strategy and simple device-manufacturing process for skin-conformable perovskite-based alternating-current electroluminescent (PeACEL) devices. These devices exhibit a narrow emission bandwidth (full-width at half-maximum, <37 nm), continuously tuneable emission wavelength (468–694 nm), high stretchability (400%) and adequate luminance (>200 cd m−2). The approach leverages a new class of perovskite zinc sulfide (PeZS) phosphors, consisting of ZnS phosphors coated with perovskite nanoparticles for electrical excitation via total intraparticle energy transfer. This strategy results in pure red and green emissions and expands the colour gamut of powder-based ACEL devices by 250%. Moreover, our processing technique facilitates the integration of PeACEL displays with wearable electronics, enabling applications in dynamic interactive displays and visual real-time temperature monitoring. These PeACEL displays offer new routes in flexible electronics and hold potential for the development of efficient artificial skins, robotics and biomedical monitoring devices.

Properties of Multistranded Twisted Graphene Fibers and Their Application in Flexible Light-Emitting Devices.

As a typical carbon-based material electrode, graphene fiber exhibits many advantages, such as good electrical conductivity, lightweight, and strong structural designability. Its demand is increasing in the wearable display field. With the help of fine denier fiber spinning combined with multistranded graphene fibers prepared via twisting and drafting, their petal-like twisted structure endows the fibers with a high specific surface area, enabling them to complete dye adsorption within 30 min. Simultaneously, compared with that of a single fiber with the same thickness, the volume specific resistance of a multistranded twisted graphene fiber is reduced by 2.4 times. During force sensing, the twisted structure of multistranded fibers exhibits varying simultaneity of fiber fracture with excellent resistance sensitivity reaching up to 55%. The multistranded twisted flexible graphene fibers demonstrate excellent robustness. Electroluminescent flexible devices prepared with graphene fibers and fiber braided fabrics with different organizational structures as electrodes emit highly saturated short-wave blue light during long-term multiple use. Therefore, multistranded twisted graphene fibers exhibit considerable potential for future applications in wearable multicolor smart displays and flexible optical signal electronics.

Modeling the electroluminescence of atomic wires from quantum dynamics simulations.

Static and time-dependent quantum-mechanical approaches have been employed in the literature to characterize the physics of light-emitting molecules and nanostructures. However, the electromagnetic emission induced by an input current has remained beyond the realm of molecular simulations. This is the challenge addressed here with the help of an equation of motion for the density matrix coupled to a photon bath based on a Redfield formulation. This equation is evolved within the framework of the driven-Liouville von Neumann approach, which incorporates open boundaries by introducing an applied bias and a circulating current. The dissipated electromagnetic power can be computed in this context from the time derivative of the energy. This scheme is applied in combination with a self-consistent tight-binding Hamiltonian to investigate the effects of bias and molecular size on the electroluminescence of metallic and semiconducting chains. For the latter, a complex interplay between bias and molecular length is observed: there is an optimal number of atoms that maximizes the emitted power at high voltages but not at low ones. This unanticipated behavior can be understood in terms of the band bending produced along the semiconducting chain, a phenomenon that is captured by the self-consistency of the method. A simple analytical model is proposed that explains the main features revealed by the simulations. The methodology, applied here at a self-consistent tight-binding level but extendable to more sophisticated Hamiltonians such as density functional tight binding and time dependent density functional theory, promises to be helpful for quantifying the power and quantum efficiency of nanoscale electroluminescent devices.

20‐1: Invited Paper: Development of Photolithgraphic Patterning of Quantum Dots for Electroluminescent Applications

In this paper the photolithgraphic patterning approaches of quantum dots in electroluminescent devices and demoes were summerized. Photolithograpy process meets the requirements for QLED mass production, including high pixel density, large‐area process and low cost. We summerized three approaches of quantum dot photolithographic procrsses, including direct photolithography, photolithography with lift‐off process and sacrificial layer assisted patterning (SLAP).

61‐3: Distinguished Paper: Realization of an Organic Semiconductor Electroluminescent Device with High Directionality and Color Purity

We are introducing an innovative organic semiconductor electroluminescent device capable of emitting light with unprecedented characteristics: high directionality (divergence angle of 1.1°) and high color purity (full width at half‐maximum of 2.5 nm). This achievement was realized through intricate design techniques aimed at enhancing gain via meticulous recombination zone control, complemented by the reduction of losses through minimizing the overlap of the optical mode with the electrodes. These groundbreaking results mark the world's first demonstration of simultaneously achieving a narrow spectrum and superior directionality in an organic electroluminescent device.

20‐3: Invited Paper: Characteristics of Cadmium‐free Blue NanoLEDs with Protection Technology Applied to Quantum Dots

The nanoLED, an electroluminescent device utilizing quantum dots (QDs), is expected to be a promising candidate for the next‐generation display. This paper presents a newly developed QD protection technology for cadmium‐free nanoLEDs that enables simultaneous achievement of high‐efficiency electroluminescence (EL) and long lifetime. The device which was prototyped by applying ZnSeTe blue QDs to an emissive layer demonstrated a maximum external quantum efficiency (EQE) of 21.0% and a luminance half‐lifetime (LT50) of 128,000 hours at 100 nits. These results indicate that cadmium‐free nanoLEDs can meet the requirements for display application in terms of both EL efficiency and reliability.

Ultraviolet electroluminescence with electrically tunable colour from epitaxial n-(0001)ZnO/p-(0001)GaN light-emitting diodes

Pulsed laser deposition technique is used to grow unintentionally n-type (0001)ZnO layers with high crystalline and morphological qualities on p-type (0001)GaN/sapphire templates. Electroluminescent devices are fabricated on these p–n heterojunctions. Oxygen pressure during growth has been found to influence strongly the crystalline and defect properties of the grown layers, which affect not only the current–voltage characteristics but also the emission properties of the electroluminescent devices. It has been observed that the electroluminescence (EL) spectra have both defects related visible and band-edge related ultraviolet (UV) transition features stemming from both GaN and ZnO sides. The study reveals that UV to visible EL intensity ratio maximizes at an optimum oxygen pressure. The relative contribution of EL originating from ZnO and GaN sides can be tuned by the applied bias, as the bias can control the depletion width and hence the carrier interdiffusion across the junction. This finding thus offers a scope to electrically tune the colour of the emitted light in these devices.

Magnetically Induced Near-Infrared Circularly Polarized Electroluminescence from an Achiral Perovskite Light-Emitting Diode

Circularly polarized electroluminescent devices are conventionally fabricated by incorporating an optically active chiral luminophore into their emission layer. Herein, we developed a circularly polarized perovskite light-emitting diode (PeLED) system with an optically inactive perovskite luminophore that can emit near-infrared circularly polarized electroluminescence (CPEL) upon application of an external magnetic field. The magnitude of the magnetic CPEL (gMCPEL) was in the order of 10−3 in the near-infrared wavelength range of 771–773 nm. Although the Pb perovskite quantum dots were achiral, the rotation direction of the CPEL of the magnetic circularly polarized PeLED system was successfully reversed by switching the Faraday geometry of the applied magnetic field. The use of achiral luminophores exhibiting magnetic-field-induced CPEL represents a new approach for the development of circularly polarized electroluminescent devices.

A light emitting device with TiO2:Er3+/ZnO heterostructure for enhanced near-infrared electroluminescence

Near-infrared (NIR) electroluminescence (EL) devices based on Er3+ ions doped TiO2 emitting layer have been fabricated by employing a facile sol–gel method. The effect of Er3+ ion doping concentration on the EL performance of TiO2:Er3+ thin film devices was investigated. Moreover, a novel device with the core of TiO2:1%Er3+/ZnO heterostructure was designed and fabricated. The EL performance of the device with optimized Er3+ ion doping concentration and improved structure was significantly improved. The NIR EL-enabling voltage of the improved device is as low as ∼5 V. The attenuated concentration quenching effect and the ZnO film as an electron blocking layer should contribute to the improved EL performance of the optimized device.

Intramolecular Sensitization Assisting High-Efficiency TADF Conjugated Polymers with Accelerating Exciton Spin Flip for Solution-Processed Electroluminescent Devices

Intramolecular Sensitization Assisting High-Efficiency TADF Conjugated Polymers with Accelerating Exciton Spin Flip for Solution-Processed Electroluminescent Devices

Fine-Tuning Crystal Structures of Lead Bromide Perovskite Nanocrystals through Trace Cadmium(II) Doping for Efficient Color-Saturated Green LEDs.

Decreasing perovskite nanocrystal size increases radiative recombination due to the quantum confinement effect, but also increases the Auger recombination rate which leads to carrier imbalance in the emitting layers of electroluminescent devices. Here, we overcome this trade-off by increasing the exciton effective mass without affecting the size, which is realized through the trace Cd2+ doping of formamidinium lead bromide perovskite nanocrystals. We observe an ~2.7 times increase in the exciton binding energy benefiting from a slight distortion of the [BX6]4- octahedra caused by doping in the case of that the Auger recombination rate is almost unchanged. As a result, bright color-saturated green emitting perovskite nanocrystals with a photoluminescence quantum yield of 96 % are obtained. Cd2+ doping also shifts up the energy levels of the nanocrystals, relative to the Fermi level so that heavily n-doped emitters convert into only slightly n-doped ones; this boosts the charge injection efficiency of the corresponding light-emitting diodes. The light-emitting devices based on those nanocrystals reached a high external quantum efficiency of 29.4 % corresponding to a current efficiency of 123 cd A-1, and showed dramatically improved device lifetime, with a narrow bandwidth of 22 nm and Commission Internationale de I'Eclairage coordinates of (0.20, 0.76) for color-saturated green emission for the electroluminescence peak centered at 534 nm, thus being fully compliant with the latest standard for wide color gamut displays.

Fine‐Tuning Crystal Structures of Lead Bromide Perovskite Nanocrystals through Trace Cadmium(II) Doping for Efficient Color‐Saturated Green LEDs

AbstractDecreasing perovskite nanocrystal size increases radiative recombination due to the quantum confinement effect, but also increases the Auger recombination rate which leads to carrier imbalance in the emitting layers of electroluminescent devices. Here, we overcome this trade‐off by increasing the exciton effective mass without affecting the size, which is realized through the trace Cd2+ doping of formamidinium lead bromide perovskite nanocrystals. We observe an ~2.7 times increase in the exciton binding energy benefiting from a slight distortion of the [BX6]4− octahedra caused by doping in the case of that the Auger recombination rate is almost unchanged. As a result, bright color‐saturated green emitting perovskite nanocrystals with a photoluminescence quantum yield of 96 % are obtained. Cd2+ doping also shifts up the energy levels of the nanocrystals, relative to the Fermi level so that heavily n‐doped emitters convert into only slightly n‐doped ones; this boosts the charge injection efficiency of the corresponding light‐emitting diodes. The light‐emitting devices based on those nanocrystals reached a high external quantum efficiency of 29.4 % corresponding to a current efficiency of 123 cd A−1, and showed dramatically improved device lifetime, with a narrow bandwidth of 22 nm and Commission Internationale de I'Eclairage coordinates of (0.20, 0.76) for color‐saturated green emission for the electroluminescence peak centered at 534 nm, thus being fully compliant with the latest standard for wide color gamut displays.