Enhanced Emitting Dipole Orientation Based on Asymmetric Iridium(III) Complexes for Efficient Saturated-Blue Phosphorescent OLEDs.

Three novel asymmetric Ir(III) complexes have been rationally designed to optimize their emitting dipole orientations (EDO) and enhance light outcoupling in blue phosphorescent organic light-emitting diodes (OLEDs), thereby boosting their external quantum efficiency (EQE). Bulky electron-donating groups (EDGs), namely: carbazole (Cz), di-tert-butyl carbazole (tBuCz), and phenoxazine (Pxz) are incorporated into the tridentate dicarbene pincer chelate to induce high degree of packing anisotropy, simultaneously enhancing their photophysical properties. Angle-dependent photoluminescence (ADPL) measurements indicate increased horizontal transition dipole ratios of 0.89 and 0.90 for the Ir(III) complexes Cz-dfppy-CN and tBuCz-dfppy-CN, respectively. Analysis of the single crystal structure and density functional theory (DFT) calculation results revealed an inherent correlation between molecular aspect ratio and EDO. Utilizing the newly obtained emitters, the blue OLED devices demonstrated exceptional performance, achieving a maximum EQE of 30.7% at a Commission International de l'Eclairage (CIE) coordinate of (0.140, 0.148). Optical transfer matrix-based simulations confirmed a maximum outcoupling efficiency of 35% due to improved EDO. Finally, the tandem OLED and hyper-OLED devices exhibited a maximum EQE of 44.2% and 31.6%, respectively, together with good device stability. This rational molecular design provides straightforward guidelines to reach highly efficient and stable saturated blue emission.

Hexacarbazolylbenzene: An Excellent Host Molecule Causing Strong Guest Molecular Orientation and the High-Performance OLEDs.

Hexacarbazolylbenzene (6CzPh), which is benzene substituted by six carbazole rings, is a simple and attractive compound. Despite the success of a wide variety of carbazole derivatives in organic light-emitting diodes (OLEDs), 6CzPh has not received attention so far. Here, excellent performances of 6CzPh are revealed as a host material in OLEDs regarding conventional host materials. Various strategies are implemented to improve the performance of OLEDs, e.g., triplet utilization by thermally activated delayed fluorescence (TADF) and phosphorescence emitters for maximizing internal quantum efficiency, and molecular orientation control for increasing outcoupling efficiency. The present host material is suited for both criteria. Robustness of the structure and sufficiently high triplet energy enables a high external quantum efficiency with a long device lifetime. Besides, the host material boosts the horizontal molecular orientations of several guest emitters. It is noteworthy that disk-shaped 4CzIPN marks the complete horizontal molecular orientations (Θh = 100%, S = -0.50). These results provide an effective way of improving efficiencies without sacrificing device durability for future OLEDs.

Buried interface modification and light outcoupling strategy for efficient blue perovskite light-emitting diodes.

Perovskite light-emitting diodes (PeLEDs) exhibit remarkable potential in the field of displays and solid-state lighting. However, blue PeLEDs, a key element for practical applications, still lag behind their green and red counterparts, due to a combination of strong nonradiative recombination losses and unoptimized device structures. In this report, we propose a buried interface modification strategy to address these challenges by focusing on the bottom-hole transport layer (HTL) of the PeLEDs. On the one hand, a multifunctional molecule, aminoacetic acid hydrochloride (AACl), is introduced to modify the HTL/perovskite interface to regulate the perovskite crystallization. Experimental investigations and theoretical calculations demonstrate that AACl can effectively reduce the nonradiative recombination losses in bulk perovskites by suppressing the growth of low-n perovskite phases and also the losses at the bottom interface by passivating interfacial defects. On the other hand, a self-assembly nanomesh structure is ingeniously developed within the HTLs. This nanomesh structure is meticulously crafted through the blending of poly-(9,9-dioctyl-fluorene-co-N-(4-butyl phenyl) diphenylamine) and poly (n-vinyl carbazole), significantly enhancing the light outcoupling efficiency in PeLEDs. As a result, our blue PeLEDs achieve remarkable external quantum efficiencies, 20.4% at 487 nm and 12.5% at 470 nm, which are among the highest reported values. Our results offer valuable insights and effective methods for achieving high-performance blue PeLEDs.

Solvent-Reconstructed Interface That Enhances Light Out-Coupling in Quasi-Two-Dimensional Perovskite Light-Emitting Diodes.

Light management is critical to maximizing the external quantum efficiency of perovskite light-emitting diodes (PeLEDs), but strategies for enhancing light out-coupling are typically complex and expensive. Here, using a facile solvent treatment strategy, we create a layer of lithium fluoride (LiF) nanoislands that serve as a template to reconstruct the light-extracting interfaces for PeLEDs. The nanoisland interface rearranges the near-field light distribution in order to maximize the efficiency of internal light extraction. With the proper adjustment of the nanoisland size and distribution, we have achieved an optimal balance between charge injection and light out-coupling, resulting in bright, pure-red quasi-two-dimensional PeLEDs with a 21.8% peak external quantum efficiency.

Optimizing Horticulture Luminescent Solar Concentrators via Enhanced Diffuse Emission Enabled by Micro-Cone Arrays.

Optimizing the photon spectrum for photosynthesis concurrently with improving crop yields presents an efficient and sustainable pathway to alleviate global food shortages. Luminescent solar concentrators (LSCs), consisting of transparent host matrices doped with fluorophores, show excellent promise to achieve the desired spectral tailoring. However, conventional LSCs are predominantly engineered for photon concentration, which results in a limited outcoupling efficiency of converted photons. Here, we introduce a scheme to implement LSCs into horticulture (HLSC) by enhancing light extraction. The symmetry of the device is disrupted by incorporating microcone arrays on the bottom surface to mitigate total internal reflection. Both Monte Carlo ray tracing simulations and experimental results have verified that the greatest enhancements in converted light extraction, relative to planar LSCs, are achieved using microcone arrays (base width 50 µm, aspect ratio 1.2) with extruded and protruded profiles (85.15 and 66.55% improvement, respectively). Angularly resolved transmission measurements show that the HLSC device exhibits a broad angular radiation distribution. This characteristic indicates that the HLSC device emits diffuse light, which is conducive to optimal plant growth.

Enhancing Light Outcoupling Efficiency via Anisotropic Low Refractive Index Electron Transporting Materials for Efficient Perovskite Light-Emitting Diodes.

Thanks to the extensive efforts toward optimizing perovskite crystallization properties, high-quality perovskite films with near-unity photoluminescence quantum yield are successfully achieved. However, the light outcoupling efficiency of perovskite light-emitting diodes (PeLEDs) is impeded by insufficient light extraction, which poses a challenge to the further advancement of PeLEDs. Here, an anisotropic multifunctional electron transporting material, 9,10-bis(4-(2-phenyl-1H-benzo[d]imidazole-1-yl)phenyl) anthracene (BPBiPA), with a low extraordinary refractive index (ne) and high electron mobility is developed for fabricating high-efficiency PeLEDs. The anisotropic molecular orientations of BPBiPA can result in a low ne of 1.59 along the z-axis direction. Optical simulations show that the low ne of BPBiPA can effectively mitigate the surface plasmon polariton loss and enhance the photon extraction efficiency in waveguide mode, thereby improving the light outcoupling efficiency of PeLEDs. In addition, the high electron mobility of BPBiPA can facilitate balanced carrier injection in PeLEDs. As a result, high-efficiency green PeLEDs with a record external quantum efficiency of 32.1% and a current efficiency of 111.7 cd A-1 are obtained, which provides new inspirations for the design of electron transporting materials for high-performance PeLEDs.

Enhancing Light Out-coupling in Perovskite Light-Emitting Diodes through Plasmonic Nanostructures.

Perovskite light-emitting diodes (PeLEDs) have emerged as promising candidates for lighting and display technologies owing to their high photoluminescence quantum efficiency and high carrier mobility. However, the performance of planar PeLEDs is limited by the out-coupling efficiency, predominantly governed by photonic losses at device interfaces. Most notably, the plasmonic loss at the metal electrode interfaces can account for up to 60% of the total loss. Here, we investigate the use of plasmonic nanostructures to improve the light out-coupling in PeLEDs. By integrating these nanostructures with PeLEDs, we have demonstrated an effectively reduced plasmonic loss and enhanced light out-coupling. As a result, the nanostructured PeLEDs exhibit an average 1.5-fold increase in external quantum efficiency and an ∼20-fold improvement in device lifetime. This finding offers a generic approach for enhancing light out-coupling, promising great potential to go beyond existing performance limitations.

Engineering the Outcoupling Pathways in Plasmonic Tunnel Junctions via Photonic Mode Dispersion for Low-Loss Waveguiding.

Outcoupling of plasmonic modes excited by inelastic electron tunneling (IET) across plasmonic tunnel junctions (TJs) has attracted significant attention due to low operating voltages and fast excitation rates. Achieving selectivity among various outcoupling channels, however, remains a challenging task. Employing nanoscale antennas to enhance the local density of optical states (LDOS) associated with specific outcoupling channels partially addressed the problem, along with the integration of conducting 2D materials into TJs, improving the outcoupling to guided modes with particular momentum. The disadvantage of such methods is that they often involve complex fabrication steps and lack fine-tuning options. Here, we propose an alternative approach by modifying the dielectric medium surrounding TJs. By employing a simple multilayer substrate with a specific permittivity combination for the TJs under study, we show that it is possible to optimize mode selectivity in outcoupling to a plasmonic or a photonic-like mode characterized by distinct cutoff behaviors and propagation length. Theoretical and experimental results obtained with a SiO2-SiN-glass multilayer substrate demonstrate high relative coupling efficiencies of (62.77 ± 1.74)% and (29.07 ± 0.72)% for plasmonic and photonic-like modes, respectively. The figure-of-merit, which quantifies the tradeoff between mode outcoupling and propagation lengths (tens of µm) for both modes, can reach values as high as 180 and 140. The demonstrated approach allows LDOS engineering and customized TJ device performance, which are seamlessly integrated with standard thin film fabrication protocols. Our experimental device is well-suited for integration with silicon nitride photonics platforms.

Enhanced Operational Stability by Cavity Control of Single-Layer Organic Light-Emitting Diodes Based on Thermally Activated Delayed Fluorescence.

Highly efficient organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) emitters are realized in recent years, but the device lifetime needs further improvement for practical display or lighting applications. In this work, a device design principle is presented by tuning the optical cavity of single-layer undoped devices, to realize efficient and long-lived TADF OLEDs. Extending the cavity length to the second-order interference maximum by increasing the emissive layer thickness broadens the recombination zone, while the optical outcoupling efficiency remains close to that of the thinner first-order devices. Such a device design leads to efficient and stable single-layer undoped OLEDs with a maximum external quantum efficiency of 16%, an LT90 of 452 h, and an LT50 of 3693 h at an initial luminance of 1000 cd m-2 , which is doubled compared to the first-order counterparts. It is further demonstrated that the widely-used empirical relation between OLED lifetime and light intensity originates from triplet-polaron annihilation, resulting in an extrapolated LT50 at 100 cd m-2 of close to 90 000 h, approaching the demands for practical backlight applications.

Fabrication of Flexible PDMS Films with Micro-Convex Structure for Light Extraction from Organic Light-Emitting Diodes.

In this study, we demonstrated organic light-emitting diodes (OLEDs) outcoupling with a flexible polydimethylsiloxane (PDMS) film with a micro-convex structure using the breath figure (BF) method. We can easily control the micro-convex pattern by adjusting the concentration of polystyrene and the humidity during the BF process. As process conditions to fabricate the micro-convex structure, polymer concentrations of 10, 20, 40, and 80 mg/mL and 60, 70, and 80% relative humidity were used. To evaluate the optical properties, we analyzed the transmission, diffusion, and electroluminescence with or without the micro-convex structure on the OLEDs. The shape and density of the micro-convex structure are related to its optical properties and outcoupling and we have experimentally demonstrated this. By applying a micro-convex structure, it achieved up to a 42% improvement in the external quantum efficiency compared to bare OLEDs (without any light extraction film). We expect the fabricated flexible light extraction film to be effective for outcoupling and applicable to flexible devices.

Patterning of Metal Halide Perovskite Thin Films and Functional Layers for Optoelectronic Applications.

In recent years, metal halide perovskites have received significant attention as materials for next-generation optoelectronic devices owing to their excellent optoelectronic properties. The unprecedented rapid evolution in the device performance has been achieved by gaining an advanced understanding of the composition, crystal growth, and defect engineering of perovskites. As device performances approach their theoretical limits, effective optical management becomes essential for achieving higher efficiency. In this review, we discuss the status and perspectives of nano to micron-scale patterning methods for the optical management of perovskite optoelectronic devices. We initially discuss the importance of effective light harvesting and light outcoupling via optical management. Subsequently, the recent progress in various patterning/texturing techniques applied to perovskite optoelectronic devices is summarized by categorizing them into top-down and bottom-up methods. Finally, we discuss the perspectives of advanced patterning/texturing technologies for the development and commercialization of perovskite optoelectronic devices.

Luminescence and Degeneration Mechanism of Perovskite Light-Emitting Diodes and Strategies for Improving Device Performance.

Perovskite light-emitting diodes (PeLEDs) can be a promising technology for next-generation display and lighting applications due to their excellent optoelectronic properties. However, a systematical overview of luminescence and degradation mechanism of perovskite materials and PeLEDs is lacking. Therefore, it is crucial to fully understand these mechanisms and further improve device performances. In this work, the fundamental photophysical processes of perovskite materials, electroluminescence mechanism of PeLEDs including carrier kinetics and efficiency roll-off as well as device degradation mechanism are discussed in detail. In addition, the strategies to improve device performances are summarized, including optimization of photoluminescence quantum yield, charge injection and recombination, and light outcoupling efficiency. It is hoped that this work can provide guidance for future development of PeLEDs and ultimately realize industrial applications.

Perovskite Light-Emitting Diodes with an External Quantum Efficiency Exceeding 30.

Perovskite light-emitting diodes (PeLEDs) are strong candidates for next-generation display and lighting technologies due to their high color purity and low-cost solution-processed fabrication. However, PeLEDs are not superior to commercial organic light-emitting diodes (OLEDs) in efficiency, as some key parameters affecting their efficiency, such as the charge carrier transport and light outcoupling efficiency, are usually overlooked and not well optimized. Here, ultrahigh-efficiency green PeLEDs are reported with quantum efficiencies surpassing a milestone of 30% by regulating the charge carrier transport and near-field light distribution to reduce electron leakage and achieve a high light outcoupling efficiency of 41.82%. Ni0.9 Mg0.1 Ox films are applied with a high refractive index and increased hole carrier mobility as the hole injection layer to balance the charge carrier injection and insert the polyethylene glycol layer between the hole transport layer and the perovskite emissive layer to block the electron leakage and reduce the photon loss. Therefore, with the modified structure, the state-of-the-art green PeLEDs achieve a world record external quantum efficiency of 30.84% (average =  29.05 ± 0.77%) at a luminance of 6514 cd m-2 . This study provides an interesting idea to construct super high-efficiency PeLEDs by balancing the electron-hole recombination and enhancing the light outcoupling.

Self-Generated Buried Submicrocavities for High-Performance Near-Infrared Perovskite Light-Emitting Diode.

Embedding submicrocavities is an effective approach to improve the light out-coupling efficiency (LOCE) for planar perovskite light-emitting diodes (PeLEDs). In this work, we employ phenethylammonium iodide (PEAI) to trigger the Ostwald ripening for the downward recrystallization of perovskite, resulting in spontaneous formation of buried submicrocavities as light output coupler. The simulation suggests the buried submicrocavities can improve the LOCE from 26.8 to 36.2% for near-infrared light. Therefore, PeLED yields peak external quantum efficiency (EQE) increasing from 17.3% at current density of 114 mA cm-2 to 25.5% at current density of 109 mA cm-2 and a radiance increasing from 109 to 487 W sr-1 m-2 with low rolling-off. The turn-on voltage decreased from 1.25 to 1.15 V at 0.1 W sr-1 m-2. Besides, downward recrystallization process slightly reduces the trap density from 8.90 × 1015 to 7.27 × 1015 cm-3. This work provides a self-assembly method to integrate buried output coupler for boosting the performance of PeLEDs.

YCl3-Substituted CsPbI3 Perovskite Nanorods for Efficient Red-Light-Emitting Diodes.

Cesium lead iodide (CsPbI3) perovskite nanocrystals (NCs) are a promising material for red-light-emitting diodes (LEDs) due to their excellent color purity and high luminous efficiency. However, small-sized CsPbI3 colloidal NCs, such as nanocubes, used in LEDs suffer from confinement effects, negatively impacting their photoluminescence quantum yield (PLQY) and overall efficiency. Here, we introduced YCl3 into the CsPbI3 perovskite, which formed anisotropic, one-dimensional (1D) nanorods. This was achieved by taking advantage of the difference in bond energies among iodide and chloride ions, which caused YCl3 to promote the anisotropic growth of CsPbI3 NCs. The addition of YCl3 significantly improved the PLQY by passivating nonradiative recombination rates. The resulting YCl3-substituted CsPbI3 nanorods were applied to the emissive layer in LEDs, and we achieved an external quantum efficiency of ~3.16%, which is 1.86-fold higher than the pristine CsPbI3 NCs (1.69%) based LED. Notably, the ratio of horizontal transition dipole moments (TDMs) in the anisotropic YCl3:CsPbI3 nanorods was found to be 75%, which is higher than the isotropically-oriented TDMs in CsPbI3 nanocrystals (67%). This increased the TDM ratio and led to higher light outcoupling efficiency in nanorod-based LEDs. Overall, the results suggest that YCl3-substituted CsPbI3 nanorods could be promising for achieving high-performance perovskite LEDs.

Research on the High Light Out-Coupling Efficiency Deep-Blue Top-Emitting Organic Light-Emitting Diode through FDTD Optical Simulation.

We have studied high light out-coupling efficiency top-emitting organic light-emitting diodes (TOLEDs) under the guidance of the finite-difference time-domain (FDTD) simulation. TOLED achieves an extraordinarily high light extraction efficiency at 468 nm, in deep-blue regions, of 49.70%, which is approximately 3.5 times that of the bottom light-emitting diode (BOLED) by changing the thickness of the organic layer and the position of the light-emitting layer in the FDTD simulation. Based on the simulation results, the TOLED with ultrahigh efficiency and narrow full width at half maximum is successfully fabricated, and the maximum external quantum efficiency of TOLED is almost 3.3 times that of the BOLED, which is perfectly consistent with the FDTD simulation results. Meanwhile, the shift of the electroluminescence spectrum of the TOLED is restricted within 10° in the angular-dependence test (0° to 80°). The optimized performance of the OLED indicates a new method to develop a high-performance device under the guidance of simulation.

Randomly Disassembled Nanostructure for Wide Angle Light Extraction of Top-Emitting Quantum Dot Light-Emitting Diodes.

The quantum dot light-emitting diode (QLED) represents one of the strongest display technologies and has unique advantages like a shallow emission spectrum and superior performance based on the cumulative studies of state-of-the-art quantum dot (QD) synthesis and interfacial engineering. However, research on managing the device's light extraction has been lacking compared to the conventional LED field. Moreover, relevant studies on top-emitting QLEDs (TE-QLEDs) have been severely lacking compared to bottom-emitting QLEDs (BE-QLEDs). This paper demonstrates a novel light extraction structure called the randomly disassembled nanostructure (RaDiNa). The RaDiNa is formed by detaching polydimethylsiloxane (PDMS) film from a ZnO nanorod (ZnO NR) layer and laying it on top of the TE-QLED. The RaDiNa-attached TE-QLED shows significantly widened angular-dependent electroluminescence (EL) intensities over the pristine TE-QLED, confirming the effective light extraction capability of the RaDiNa layer. Consequently, the optimized RaDiNa-attached TE-QLED achieves enhanced external quantum efficiency (EQE) over the reference device by 60%. For systematic analyses, current-voltage-luminance (J-V-L) characteristics are investigated using scanning electron microscopy (SEM) and optical simulation based on COMSOL Multiphysics. It is believed that this study's results provide essential information for the commercialization of TE-QLEDs.

Enhanced performance of organic light-emitting diodes by integrating quasi-periodic micro-nano structures.

To integrate a quasi-periodic micro-nano structure (PMS) to the organic light-emitting devices (OLEDs) is an efficient way to enhance the performance of OLEDs. In this paper, the PMS prepared by the phase separation of Polystyrene and Poly (methyl methacrylate) was integrated to the OLEDs with the structures of Glass/PMS/Ag (30 nm)/MoO3 (5 nm)/(NPB) (40 nm)/(Alq3) (60 nm)/LiF (0.5 nm)/Al (150 nm). The maximum luminance intensity and external quantum efficiency increased to 10700 cd/m2 and 1.11 %, which is 48 % and 44 % higher than that of 7209 cd/m2 and 0.77 % of the planar reference device. The enhanced performance of OLEDs was ascribed to the attenuation of surface plasmon polariton loss caused by the PMS, which was testified by the Finite-Difference Time-Domain (FDTD) simulation. The PMS was also transferred to the hole transfer layer (PEDOT: PSS) of OLEDs by nano-imprinting lithography with the structure of Glass/(ITO) (100 nm)/PEDOT: PSS (100 nm) (with PMS)/NPB (10 nm)/Alq3 (50 nm)/LiF (0.5 nm)/Al (100 nm). The performance was also improved by the optimized PMS and the light out-coupling efficiency increased to about 49.5 %, which is much higher than that of 28.8 % in the OLEDs with PMS Ag anode and 20 % in the planar reference devices. This suggests that the PMS can improve the OLED device performance regardless of the functional layer in which the PMS is integrated.

Improving Electroluminescence Efficiency by Linear Polar Host Capable of Promoting Horizontal Dipole Orientation for Dopant.

In doped organic light-emitting diodes (OLEDs), the host materials play an important role in emitting layers. Most studies about host materials mainly focus on their energy levels and carrier transport behaviors, while less attention is paid to their influence on the dipole orientation of dopants, which closely associate with the light out-coupling efficiency (ηout ) of the device. Herein, a linear polar host material (l-CzTRZ) consisting of carbazole donor, triazine acceptor, and the conjugated para-terphenyl skeleton is developed and its crystal and electronic structures, thermal and electrochemical stabilities, optical property, and carrier transport ability are investigated. l-CzTRZ prefers ordered horizontal orientation and favors electron transport in neat film. More importantly, it can promote horizontal dipole orientation for the dopants via dipole-dipole interaction, furnishing an excellent horizontal dipole ratio of 91.5% and thus a high ηout of 43% for the phosphorescent dopant (PO-01-TB). Consequently, the OLED with l-CzTRZ host and PO-01-TB dopant attains state-of-the-art electroluminescence efficiencies of 135.5 cd A-1 , 135.7 lm W-1 and 41.3%, with a small roll-off of 9.7% at 5000 cd m-2 luminance. The presented significant impact of the host on the dipole orientation of the dopant shall enlighten the design of host materials to improve OLED performance.

Polymer Dispersed Liquid Crystal Imprinted by Microlens Array for Enhanced Outcoupling Efficiency of Organic Light Emitting Diode.

In this paper, we demonstrate the use of polymer dispersed liquid crystal (PDLC) imprinted with a microlens array (MLA) via solution process to improve the outcoupling efficiency of organic light emitting diodes (OLEDs). The PDLC, well known for its scattering effect, is an excellent technology for improving the outcoupling efficiency of OLEDs. Additionally, we introduce a simple spin-coating process to fabricate PDLC which is adaptable for future solution-processed OLEDs. The MLA-imprinted PDLC applied OLED shows an enhancement factor of 1.22 in outcoupling efficiency which is a 37.5% increase compared to the existing PDLC techniques without changing the electrical properties of the OLED. Through this approach, we can expect the roll-to-roll based extremely flexible OLED, and with further research on pattering PDLC by various templates, higher outcoupling efficiency is achievable through a simple UV irradiation process.