Efficient Perovskite Light-emitting Diodes Research Articles

Efficient All-Inorganic Perovskite Light-Emitting Diodes Enabled by Simultaneous Growth Regulation and Defect Passivation

Efficient All-Inorganic Perovskite Light-Emitting Diodes Enabled by Simultaneous Growth Regulation and Defect Passivation

Surface-binding molecular multipods strengthen the halide perovskite lattice and boost luminescence

Reducing the size of perovskite crystals to confine excitons and passivating surface defects has fueled a significant advance in the luminescence efficiency of perovskite light-emitting diodes (LEDs). However, the persistent gap between the optical limit of electroluminescence efficiency and the photoluminescence efficiency of colloidal perovskite nanocrystals (PeNCs) suggests that defect passivation alone is not sufficient to achieve highly efficient colloidal PeNC-LEDs. Here, we present a materials approach to controlling the dynamic nature of the perovskite surface. Our experimental and theoretical studies reveal that conjugated molecular multipods (CMMs) adsorb onto the perovskite surface by multipodal hydrogen bonding and van der Waals interactions, strengthening the near-surface perovskite lattice and reducing ionic fluctuations which are related to nonradiative recombination. The CMM treatment strengthens the perovskite lattice and suppresses its dynamic disorder, resulting in a near-unity photoluminescence quantum yield of PeNC films and a high external quantum efficiency (26.1%) of PeNC-LED with pure green emission that matches the Rec.2020 color standard for next-generation vivid displays.

The Crystallization Regulation Effect of the Phenyl Ring of Passivators for Blue Perovskite Light-Emitting Diodes.

Although metal halide perovskites (MHPs) have demonstrated remarkable external quantum efficiencies (EQEs) in red and green light-emitting diodes (LEDs), the blue ones confront efficiency and stability problems due to the high defect density in the perovskite films. Large amounts of defect passivation strategies are successfully developed to improve the device performance. Nevertheless, the influence of the molecular configuration of the passivators on the perovskite crystallization process has not been comprehensively investigated so far. Here, we investigate the effect of the phenyl ring on the perovskite crystallization dynamics and the passivation effect. The additive with a phenyl ring performs the π-π stacking ability with phenethylammonium (PEA+) molecules, resulting in a deteriorated crystallinity and a weakened passivation ability. Conversely, the additive without the phenyl ring is helpful to promote the participation of PEA+ molecules in the crystalline process, leading to a higher crystallinity and a stronger passivation effect. As a result, the EQE of the blue perovskite LED has increased from 4.72 to 11.06% by using the phenyl ring-free additive. Therefore, it is advisible to develop the conjugated nonplanar additives in the PEA+-assisted quasi-two-dimensional perovskites. This finding may enlighten the rational design of defect passivators for highly efficient perovskite LEDs.

Monoammonium Modified Dion-Jacobson Quasi-2D Perovskite for High Efficiency Pure-Blue Light Emitting Diodes.

Quasi-2D perovskites exhibit impressive optoelectronic properties and hold significant promise for future light-emitting devices. However, the efficiency of perovskite light-emitting diodes (PeLEDs) is seriously limited by defect-induced nonradiative recombination and imbalanced charge injection. Here, the defect states are passivated and charge injection balance is effectively improved by introducing the additive cyclohexanemethylammonium (CHMA) to bromide-based Dion-Jacobson (D-J) structure quasi-2D perovskite emission layer. CHMA participates in the crystallization of perovskite, leading to high quality film composed of compact and well-contacted grains with enhanced hole transportation and less defects. As a result, the corresponding PeLEDs exhibit stable pure blue emission at 466nm with a maximum external quantum efficiency (EQE) of 9.22%. According to current knowledge, this represents the highest EQE reported for pure-blue PeLEDs based on quasi-2D bromide perovskite thin films. These findings underscore the potential of quasi-2D perovskites for advanced light-emitting devices and pave the way for further advancements in 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.

Chelation strategy induced blue-shift for efficient deep-blue perovskite light-emitting diodes

Chelation strategy induced blue-shift for efficient deep-blue perovskite light-emitting diodes

Acceleration of radiative recombination for efficient perovskite LEDs

The increasing demands for more efficient and brighter thin-film light-emitting diodes (LEDs) in flat-panel display and solid-state lighting applications have promoted research into three-dimensional (3D) perovskites. These materials exhibit high charge mobilities and low quantum efficiency droop1–6, making them promising candidates for achieving efficient LEDs with enhanced brightness. To improve the efficiency of LEDs, it is crucial to minimize nonradiative recombination while promoting radiative recombination. Various passivation strategies have been used to reduce defect densities in 3D perovskite films, approaching levels close to those of single crystals3. However, the slow radiative (bimolecular) recombination has limited the photoluminescence quantum efficiencies (PLQEs) of 3D perovskites to less than 80% (refs. 1,3), resulting in external quantum efficiencies (EQEs) of LED devices of less than 25%. Here we present a dual-additive crystallization method that enables the formation of highly efficient 3D perovskites, achieving an exceptional PLQE of 96%. This approach promotes the formation of tetragonal FAPbI3 perovskite, known for its high exciton binding energy, which effectively accelerates the radiative recombination. As a result, we achieve perovskite LEDs with a record peak EQE of 32.0%, with the efficiency remaining greater than 30.0% even at a high current density of 100 mA cm−2. These findings provide valuable insights for advancing the development of high-efficiency and high-brightness perovskite LEDs.

Efficient pure-red perovskite light-emitting diodes with strong passivation via ultrasmall-sized molecules.

Perovskite light-emitting diodes (PeLEDs) have attracted great attention in recent years; however, the halogen vacancy defects in perovskite notably hamper the development of high-efficiency devices. Previously, large-sized passivation agents have been usually used, while the effect of defect passivation is limited due to the weak bonding or the large space steric hindrance. Here, we predict that the ultrasmall-sized formate (Fa) and acetate (Ac) have more efficient passivation ability because of the stronger binding with the perovskite, as demonstrated by density functional theory calculation. We introduce ultrasmall-sized cesium salts (CsFa/CsAc) into buried interface, which can also diffuse into the bulk, resulting in both buried interface and bulk passivation. In addition, the improved perovskite growth has been found due to the enhanced hydrophily after introducing CsFa/CsAc as additive. According to these advantages, a pure-red PeLED with 24.2% efficiency at 639 nm has been achieved.

Vertically Concentrated Quantum Wells Enabling Highly Efficient Deep-Blue Perovskite Light-Emitting Diodes.

Deep-blue perovskite light-emitting diodes (PeLEDs) based on quasi-two-dimensional (quasi-2D) systems exist heightened sensitivity to the domain distribution. The top-down crystallization mode will lead to a vertical gradient distribution of quantum well (QW) structure, which is unfavorable for deep-blue emission. Herein, a thermal gradient annealing treatment is proposed to address the polydispersity issue of vertical QWs in quasi-2D perovskites. The formation of large-n domains at the upper interface of the perovskite film can be effectively inhibited by introducing a low-temperature source in the annealing process. Combined with the utilization of NaBr to inhibit the undesirable n=1 domain, a vertically concentrated QW structure is ultimately attained. As a result, the fabricated device delivers a narrow and stable deep-blue emission at 458 nm with an impressive external quantum efficiency (EQE) of 5.82 %. Green and sky-blue PeLEDs with remarkable EQE of 21.83 % and 17.51 % are also successfully achieved, respectively, by using the same strategy. The findings provide a universal strategy across the entire quasi-2D perovskites, paving the way for future practical application of PeLEDs.

Regulating Surface-Passivator Binding Priority for Efficient Perovskite Light-Emitting Diodes.

Suppressing trap-assisted nonradiative losses through passivators is a prerequisite for efficient perovskite light-emitting diodes (PeLEDs). However, the complex bonding between passivators and perovskites severely suppresses the passivation process, which still lacks comprehensive understanding. Herein, the number, category, and degree of bonds between different functional groups and the perovskite are quantitatively assessed to study the passivation dynamics. Functional groups with high electrostatic potential and large steric hindrance prioritize strong bonding with organic cations and halides on the perfect surface, leading to suppressed coordination with bulky defects. By modulating the binding priorities and coordination capacity, hindrance from the intense interaction with perfect perovskite is significantly reduced, leading to a more direct passivation process. Consequently, the near-infrared PeLED without external light out-coupling demonstrates a record external quantum efficiency of 24.3% at a current density of 42mA cm-2. In addition, the device exhibits a record-level-cycle ON/OFF switching of 20000 and ultralong half-lifetime of 1126.3h under 5mA cm-2. An in-depth understanding of the passivators can offer new insights into the development of high-performance 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 111.7cd A-1 are obtained, which provides new inspirations for the design of electron transporting materials for high-performance PeLEDs.

Suppressing interfacial nonradiative recombination by alkali hydroxides for efficient blue perovskite light-emitting diodes

Blue perovskite light-emitting diodes (PeLEDs) provide unlimited possibility in the field of optoelectronic devices due to their excellent characteristics. However, the widely used hole-transport material, poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), has strong acidity and poor conductivity which deteriorate the efficiency and stability of perovskite devices. In this work, we modified PEDOT:PSS layer using alkalis, LiOH, NaOH, and KOH, to address these issues. Our findings indicated that the indium defect from indium tin oxide substrate was passivated after the introduction of LiOH, which resulted in the suppression of nonradiative recombination. In addition, the conductivity was improved owing to the increased phase separation of PEDOT:PSS. Taking advantage of optimized interface, the small-n phases of quasi-two-dimensional (quasi-2D) perovskite films were redistributed in quantities and dimensions. As results of these improvements, blue PeLEDs possessed the external quantum efficiencies of 5.95 % and an extended half-lifetime with emission-light wavelength of 473 nm. These findings offer an effective strategy to achieve highly efficient blue light-emitting diode.

High brightness and low operating voltage CsPbBr3 perovskite LEDs by single-source vapor deposition

In this work, we utilized CsPbBr3 powder as the precursor material for the single-source vapor deposition (SSVD) process to fabricate the CsPbBr3 emitting layer. Due to the high density of grain boundaries and defects in the thin films deposited in the initial stages, non-radiative recombination can occur, reducing the efficiency of perovskite light-emitting diodes (PeLED). To address this issue, we employed a thermal annealing process by subjecting the perovskite films to the appropriate annealing temperature, facilitating the coalescence and growth of different grains, improving lattice integrity, and thereby reducing the presence of defects and enhancing the photoluminescence performance of the films. Furthermore, in this study, we successfully fabricated simple-structured CsPbBr3 PeLED using thermally annealed CsPbBr3 films. Among these components, even without adding the electron and hole transport layers, the best-performing device achieved a maximum brightness of 14,079 cd/m2 at a driving voltage of only 2.92 V after annealing at 350 °C; the brightness is 16.8 times higher than that of CsPbBr3 PeLED without heat treatment, demonstrating outstanding light-emitting performance. The research results show that using SSVD to prepare CsPbBr3 PeLED has broad application potential, providing a simple process option for research on improving the performance of PeLED.

Self-assembled mono-hole-injecting layers towards efficient deep-blue perovskite light-emitting diodes

Hole-injection layers (HILs) play crucial roles in enhancing the performance of perovskite light-emitting diodes (PeLEDs) by lowering the energy barrier between the anode and the hole-transport layer (HTL). However, the commonly employed HIL, poly(3,4-ethylenedioxythiophene): polystyrene sulfonic acid (PEDOT: PSS) has notable drawbacks, such as extreme acidity and susceptibility to corrosion, which severely hampers device efficiency and stability. Herein, a self-assembled monolayer (SAM)-[2-(9H-Carbazol-9-yl) ethyl] phosphonic acid (2PACz) instead of PEDOT: PSS was employed in PeLEDs, which could reduce the negative impacts on neighboring perovskite sites and indium tin oxide electrodes. To obtain favorable energy level alignment between 2PACz and the perovskite layer, poly(9-vinylcarbazole) (PVK) was introduced as an indispensable HTL. Consequently, the 2PACz/PVK-based deep-blue PeLEDs exhibit a lower turn-on voltage of 3.20 V, and a peak external quantum efficiency of 4.42 % at 467 nm, which is a threefold improvement over the control devices. This impressive performance boost can be attributed to the reduction in interfacial defects and the improved balance of carrier injection, leading to more efficient light emission. Our study not only introduces an innovative and cost-effective HIL solution for PeLEDs but also provides valuable insights and guidance for the development of highly efficient and stable PeLEDs in the future.

Phase dimensions resolving of efficient and stable perovskite light-emitting diodes at high brightness

Phase dimensions resolving of efficient and stable perovskite light-emitting diodes at high brightness

Interface engineering with ionic liquid for achieving efficient Quasi-2D perovskite light-emitting diodes

Perovskite light-emitting diodes (PeLEDs) have attracted wide attention due to their excellent photoelectric properties. A variety of additives have been studied for perovskite emission layers to enhance the performance of PeLEDs. However, the buried interface, which also has significant influence on the crystallization kinetics and exciton recombination dynamics of the perovskite emission layer, remains to be explored. In this work, we introduced a new ionic liquid 1-Ethyl-3-methylimidazolium dicyanamide (EMIM DCA) with the characteristics of low viscosity and high conductivity into the interfacial layer between the hole transport layer (HTL) and the perovskite film. Due to the strong interaction between the EMIM DCA and perovskite, the crystallization of the perovskite film is obviously improved and the defects at the interface are well passivated. As a result, the nonradiative recombination in the interlayer is significantly reduced. In addition, the introduction of EMIM DCA promoted the injection of charge carriers, thus achieving a high luminance of 32310 cd m−2 and enabling the maximum external quantum efficiency (EQE) of the PeLEDs increased from 10.2 % to 18.7 %.

Stable and Efficient Mixed-halide Perovskite LEDs.

Tailoring bandgap by mixed-halide strategy in perovskites has attracted extraordinary attention due to the flexibility of halide ion combinations and has emerged as the most direct and effective approach to precisely tune the emission wavelength throughout the entire visible light spectrum. Mixed-halide perovskites, yet, still suffered from several problems, particularly phase segregation under external stimuli because of ions migration. Understanding the essential cause and finding sound strategies, thus, remains a challenge for stable and efficient mixed-halide perovskite light-emitting diodes (PeLEDs). The review herein presents an overview of the diverse application scenarios and the profound significance associated with mixed-halide perovskites. We then summarize the challenges and potential research directions toward developing high stable and efficient mixed-halide PeLEDs. The review thus provides a systematic and timely summary for the community to deepen the understanding of mixed-halide perovskite materials and resulting PeLEDs.

A 3D simulation model to study all-inorganic CsPbX3 (X = Br and I) perovskites-based light-emitting diodes with different hole-transporting layers

The development of numerical models is essential for optimizing perovskite light-emitting diodes (PeLEDs) and explaining their physical mechanism for further efficiency improvement. This study reports, for the first time, on a detailed device modelling of an all-inorganic perovskite LED consisting of CsPbX3 (X = Br and I) as light emitting layer (LEL) with different hole transporting layers (HTLs), employing COMSOL Multiphysics simulation package. Therefore, a 3D simulation model is served to investigate the appropriate HTLs that meet the design requirements of a PeLED in terms of band off-set engineering. For this purpose, a series of all-inorganic halide perovskites with different HTLs such as PEDOT: PSS, CuSCN and MoO3 are simulated under the same theoretical settings, and the performances of LEDs are compared with each other. This is done through studying their electronic properties using current density–voltage (J-V) curves and internal quantum efficiency (IQE) measurements. The results obtained from the J-V curves reveal that all the CsPbBr3-based samples with different HTLs exhibit the same turn-on voltage (V on) of approximately 4.2 V, while this value increases to 5.8 V for the CsPbI3-based samples. Compared with the PeLEDs based on CsPbI3, the PeLEDs based on CsPbBr3 indicate lower V on due to the formation of shorter charge carrier injection barriers at their interfaces. Furthermore, among the various simulated structures, the highest IQE is obtained for perovskite CsPbI3-based LED with MoO3 HTL (5.21%). The effect of different parameters on the performance of the proposed configurations are also investigated, and it turns out that the thickness of LELs and lifetime of charge carriers have a decisive role to play in the efficiency of PeLEDs. This theoretical study not only successfully explains the working principle of PeLEDs but also clearly shows researchers how to produce high-performance LEDs in the laboratory by knowing the physical properties of materials and accurately adjusting energy band alignments.

Co-regulation strategy dominated by double short molecules permitting the regrowth of quantum dots for efficient deep-blue perovskite light-emitting diodes

Recently, blue perovskite quantum dots (PeQDs) have garnered considerable attention for use in full-color optoelectronic displays. However, the large specific surface area caused by the small particle size of blue PeQDs results in high defect state density, which severely limits their optical pursuit. To address this issue, a co-regulation strategy using double short-chain molecules of tetraoctylammonium fluoride and tetraethylammonium perfluorooctanesulfonate is proposed to enhance the regrowth of blue CsxRb1−xPb(ClyBr1−y)3 PeQDs. Long-chain insulated oleylamine and oleic acid ligands, which restrict the growth of PeQDs, are substantially replaced using short-chain ligands with higher adsorption energy. This replacement promotes PeQDs to regrow considerably from ∼8 to ∼18 nm, and the defect-state density decreases by 3–5 times. Consequently, highly efficient blue PeQDs with a photoluminescent quantum yield of unity are obtained. Moreover, the PeQDs exhibit lower insulating ligand density and improved charge injection property. As a result, the synthesized deep-blue PeQD light-emitting diodes (PeQLEDs) exhibit a maximum external quantum efficiency of 5.7% at the CIE coordinate of (0.148, 0.032). According to the International Telecommunication Union Radiocommunication Sector television standard (Rec. 2100), the obtained PeQLEDs are state-of-the-art among colloidal deep-blue PeQDs. This study provides a novel strategy to improve the optical performance of deep-blue PeQLEDs and paves the way for developing high-end wide color-gamut displays.

Effective Small Organic Molecule as a Defect Passivator for Highly Efficient Quasi-2D Perovskite Light-Emitting Diodes.

The use of a small organic molecular passivator is proven to be a successful strategy for producing higher-performing quasi-2D perovskite light-emitting diodes (PeLEDs). The small organic molecule can passivate defects on the grain surround and surface of perovskite crystal structures, preventing nonradiative recombination and charge trapping. In this study, a new small organic additive called 2, 8-dibromodibenzofuran (diBDF) is reported and examines its effectiveness as a passivating agent in high-performance green quasi-2D PeLEDs. The oxygen atom in diBDF, acting as a Lewis base, forms coordination bonds with uncoordinated Pb2+, so enhancing the performance of the device. In addition, the inclusion of diBDF in the quasi-2D perovskite results in a decrease in the abundance of low-n phases, hence facilitating efficient carrier mobility. Consequently, PeLED devices with high efficiency are successfully produced, exhibiting an external quantum efficiency of 19.9% at the emission wavelength of 517 nm and a peak current efficiency of 65.0 cd A-1.