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.

Increasing Photoluminescence Quantum Yield by Nanophotonic Design of Quantum-Confined Halide Perovskite Nanowire Arrays.

High-photoluminescence quantum yield (PLQY) is required to reach optimal performance in solar cells, lasers, and light-emitting diodes (LEDs). Typically, PLQY can be increased by improving the material quality to reduce the nonradiative recombination rate. It is in principle equally effective to improve the optical design by nanostructuring a material to increase light out-coupling efficiency (OCE) and introduce quantum confinement, both of which can increase the radiative recombination rate. However, increased surface recombination typically minimizes nanostructure gains in PLQY. Here a template-guided vapor phase growth of CH3NH3PbI3 (MAPbI3) nanowire (NW) arrays with unprecedented control of NW diameter from the bulk (250 nm) to the quantum confined regime (5.7 nm) is demonstrated, while simultaneously providing a low surface recombination velocity of 18 cm s-1. This enables a 56-fold increase in the internal PLQY, from 0.81% to 45.1%, and a 2.3-fold increase in OCEy to increase the external PLQY by a factor of 130, from 0.33% up to 42.6%, exclusively using nanophotonic design.

Engineering light outcoupling in 2D materials.

When light is incident on 2D transition metal dichalcogenides (TMDCs), it engages in multiple reflections within underlying substrates, producing interferences that lead to enhancement or attenuation of the incoming and outgoing strength of light. Here, we report a simple method to engineer the light outcoupling in semiconducting TMDCs by modulating their dielectric surroundings. We show that by modulating the thicknesses of underlying substrates and capping layers, the interference caused by substrate can significantly enhance the light absorption and emission of WSe2, resulting in a ∼11 times increase in Raman signal and a ∼30 times increase in the photoluminescence (PL) intensity of WSe2. On the basis of the interference model, we also propose a strategy to control the photonic and optoelectronic properties of thin-layer WSe2. This work demonstrates the utilization of outcoupling engineering in 2D materials and offers a new route toward the realization of novel optoelectronic devices, such as 2D LEDs and solar cells.

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.

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.

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.

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.

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.

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.

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.

Solution-Processed Red, Green, and Blue Quantum Rod Light-Emitting Diodes.

Solution-processed semiconductor nanocrystals are evolving as potential candidates for future display and lighting applications owing to their size-tunable emission, ultrasaturated colors, and compatibility with large-area flexible substrates. Among them, quantum rods (QRs) are emerging materials for optoelectronic applications, offering polarized emission, high light outcoupling efficiency, color purity, and better stability in solid films. However, synthesizing QRs covering the full visible wavelength region has been a big challenge, particularly in the blue range. Herein, we report for the first time the synthesis of red CdSe/CdS, green CdSe/ZnxCd1-xS/ZnS, and blue CdSe/ZnxCd1-xS/ZnS QRs and their application in red, green, and blue QR-based light-emitting diodes (QR-LEDs). We have improved the charge injection balance into the QRs through embedding a poly(methyl methacrylate) (PMMA) layer between the emissive and electron transport layers. The thin PMMA electron-blocking layer (EBL) suppresses the excessive electron flux and thus promotes charge injection balance and pushes the recombination zone back to the QR layer, resulting in 1.35×, 1.2×, and 1.7× peak external quantum efficiency improvement for red, green, and blue QR-LEDs, respectively. The efficiency roll-off of green and blue QR-LEDs with an EBL is less than 50% at maximum current density. The proposed red, green, and blue QR-LEDs open up an avenue toward further improving the light source efficiency and stability focusing on real device applications.

Nanopatterning of Perovskite Thin Films for Enhanced and Directional Light Emission.

Lead-halide perovskites offer excellent properties for lighting and display applications. Nanopatterning perovskite films could enable perovskite-based devices with designer properties, increasing their performance and adding novel functionalities. We demonstrate the potential of nanopatterning for achieving light emission of a perovskite film into a specific angular range by introducing periodic sol-gel structures between the injection and emissive layer by using substrate conformal imprint lithography (SCIL). Structural and optical characterization reveals that the emission is funnelled into a well-defined angular range by optical resonances, while the emission wavelength and the structural properties of the perovskite film are preserved. The results demonstrate a flexible and scalable approach to the patterning of perovskite layers, paving the way toward perovskite LEDs with designer angular emission patterns.

Advances in Perovskite Light-Emitting Diodes Possessing Improved Lifetime.

Recently, perovskite light-emitting diodes (PeLEDs) are seeing an increasing academic and industrial interest with a potential for a broad range of technologies including display, lighting, and signaling. The maximum external quantum efficiency of PeLEDs can overtake 20% nowadays, however, the lifetime of PeLEDs is still far from the demand of practical applications. In this review, state-of-the-art concepts to improve the lifetime of PeLEDs are comprehensively summarized from the perspective of the design of perovskite emitting materials, the innovation of device engineering, the manipulation of optical effects, and the introduction of advanced encapsulations. First, the fundamental concepts determining the lifetime of PeLEDs are presented. Then, the strategies to improve the lifetime of both organic-inorganic hybrid and all-inorganic PeLEDs are highlighted. Particularly, the approaches to manage optical effects and encapsulations for the improved lifetime, which are negligibly studied in PeLEDs, are discussed based on the related concepts of organic LEDs and Cd-based quantum-dot LEDs, which is beneficial to insightfully understand the lifetime of PeLEDs. At last, the challenges and opportunities to further enhance the lifetime of PeLEDs are introduced.

Deep Blue Fluorescent Material with an Extremely High Ratio of Horizontal Orientation to Enhance Light Outcoupling Efficiency (44%) and External Quantum Efficiency in Doped and Non-Doped Organic Light-Emitting Diodes.

A novel bis-4Ph-substituted 9,10-dipehnylanthracene deep blue [1931 CIE (0.15, 0.08)] fluorescent compound, AnB4Ph, has been synthesized and characterized for organic light-emitting diode (OLED) applications. Our experimental study of AnB4Ph excludes the possibility of triplet-triplet annihilation, hybridized local and charge transfer, or thermally activated delayed fluorescent characteristics of the material. Since the solid-state photoluminescence quantum yield of AnB4Ph was determined to be 48%, assuming a 100% for the charge recombination efficiency, the light outcoupling efficiency (ηout) of an AnB4Ph non-doped OLED achieving an external quantum efficiency (EQE) of 5.3% is at least 44%, which is more than twofold higher than 20% for conventional OLEDs. Both grazing incidence wide-angle X-ray scattering (GIWAXS) and angle-dependent photoluminescence (ADPL) measurements reveal AnB4Ph having a high value of order parameter (SGIWAXS) of 0.61 for a ππ stacking along the normal direction and an orientation order parameter (SADPL) for a horizontal emitting dipole moment of -0.50 or Θ (horizontal-dipole ratios) of 100%, respectively. Otherwise, a refractive index (n) measurement provides a n = 1.80 for AnB4Ph thin films. Based on ηout = 1.2 × n-2, the calculated ηout is 37%, which is also in accordance with the results of GIWAXS and ADPL. We have also fabricated the classical fluorescent DPAVBi-doped AnB4Ph OLEDs, which display a true blue [1931 CIE (0.15 and 0.16)] electroluminescence with a high efficiency (EQE = 6.9%), surpassing the conventional ∼5% EQE. Based on an ηout of 42% for DPAVBi-doped AnB4Ph OLEDs, our studies suggest that the extremely horizontally aligned AnB4Ph host material exerts the same horizontal alignment on the DPAVBi dopant molecules.

Improving the Performance of Blue Polymer Light-Emitting Diodes Using a Hole Injection Layer with a High Work Function and Nanotexture.

For light-emitting polymers with a deep highest occupied molecular orbital energy level used for polymer light-emitting diodes (PLEDs), the hole injection barrier and hole transport of the anode buffer layer are of vital importance for optimizing electroluminescent performance. In this study, high-work-function hole injection layers with nanotextures were achieved by modifying poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) with a perfluorinated ionomer (PFI) and n-butyl alcohol and were used to achieve a single-layer device without a hole transport layer. With such an interlayer, the PLEDs based on PPF-SO25 exhibit remarkable current efficiency over 13.0 cd A-1, which significantly outperform the devices with regular PEDOT:PSS. To our knowledge, this performance is among the best reported for single-layer blue PLEDs. The bias-dependent capacitance curves of these PLEDs suggest a nonuniform surface distribution of PFI. Our findings show that the PFI-modified PEDOT:PSS not only operates as a high-work-function hole injection layer to facilitate hole injection but also as a potential inner scattering medium for light extraction.

Molecular Orientations of Delayed Fluorescent Emitters in a Series of Carbazole-Based Host Materials.

Molecular orientation is one of the most crucial factors to boost the efficiency of organic light-emitting devices. However, active control of molecular orientation of the emitter molecule by the host molecule is rarely realized so far, and the underlying mechanism is under discussion. Here, we systematically investigated the molecular orientations of thermally activated delayed fluorescence (TADF) emitters in a series of carbazole-based host materials. Enhanced horizontal orientation of the TADF emitters was achieved. The degree of enhancement observed was dependent on the host material used. Consequently, our results indicate that π-π stacking, CH/n (n = O, N) weak hydrogen bonds, and multiple CH/π contacts greatly induce horizontal orientation of the TADF emitters in addition to the molecular shape anisotropy. Finally, we fabricated TADF-based organic light-emitting devices with an external quantum efficiency (ηext) of 26% using an emission layer with horizontal orientation ratio (Θ) of 79%, which is higher than that of an almost randomly oriented emission layer with Θ of 62% (ηext = 22%).

High-Efficiency Perovskite Light-Emitting Diodes with Improved Interfacial Contact.

Unbalanced charge injection is one of the major issues that hampers the efficiency of perovskite light-emitting diodes (PeLEDs). Through engineering the device structure with multiple hole transport layers (HTLs), i.e., poly(9,9-dioctyl-fluorene-co-N-(4-butylphenyl)diphenylamine) (TFB)/poly(9-vinylcarbazole) (PVK) and nickel oxide (NiOx)/TFB/PVK, efficient PeLED devices have been successfully demonstrated. However, in a typical solution-processed PeLED with multiple HTLs, the underlying conjugated HTL could be easily redissolved by the ink of the following one, which not only dramatically deteriorates the electrical property of HTLs but also influences the quality of the top perovskite films. In this work, through inserting a thin atomic layer-deposited aluminum oxide (Al2O3) layer between HTLs and the perovskite layer, an improved interfacial contact can be achieved, which enables us to obtain perovskite films with enhanced characteristics and balanced charge injection in the resultant PeLEDs. In addition, because of the proper refractive index (r), the presence of the Al2O3 layer also favors the light out-coupling of PeLEDs. As a result, we fabricate green PeLEDs with good repeatability and external quantum efficiency of 17.0%, which is approximately 60% higher than that of the control device without Al2O3. Our work provides a promising avenue to enhance interfacial contact between the charge transport layer and perovskite for efficient perovskite-based optoelectronic devices.

Rational Interface Engineering for Efficient Flexible Perovskite Light-Emitting Diodes.

Although perovskite light-emitting diodes (PeLEDs) are promising for next-generation displays and lighting, their efficiency is still considerably below that of conventional inorganic and organic counterparts. Significant efforts in various aspects of the electroluminescence process are required to achieve high-performance PeLEDs. Here, we present an improved flexible PeLED structure based on the rational interface engineering for energy-efficient photon generation and enhanced light outcoupling. The interface-stimulated crystallization and defect passivation of the perovskite emitter are synergistically realized by tuning the underlying interlayer, leading to the suppression of trap-mediated nonradiative recombination losses. Besides approaching highly emissive perovskite layers, the outcoupling of trapped light is also enhanced by combining the silver nanowires-based electrode with quasi-random nanopatterns on flexible plastic substrate. Upon the collective optimization of the device structure, a record external quantum efficiency of 24.5% is achieved for flexible PeLEDs based on green-emitting CsPbBr3 perovskite.