Stable Perovskite Light-emitting Diodes Research Articles

Conjugated Polyelectrolytes as a Defect-Passivating Hole Injection Layer for Efficient and Stable Perovskite Light-Emitting Diodes

Conjugated Polyelectrolytes as a Defect-Passivating Hole Injection Layer for Efficient and Stable Perovskite Light-Emitting Diodes

Mitigating bulk halide defects in blue-emissive perovskite nanocrystals using benzoyl halides for efficient light-emitting diodes

While recent advances have demonstrated highly efficient and stable perovskite light-emitting diodes (LEDs), blue perovskite LEDs still show low performance compared to green, red, near IR counterparts. Despite perovskites being well-known for their defect tolerance, blue perovskites are highly vulnerable to defects, which introduce deep trap states. In this study, we mitigated bulk halide vacancies in perovskite nanocrystals (PNCs) via the diffusion-assisted halide repairing strategy. We confirmed halide vacancies inside as-synthesized PNCs, both in the core and on the surface, through HADDF-STEM. By treating PNCs with benzoyl halides, these halide vacancies were further mitigated due to halide diffusion via concentration gradients between the surface and the core, resulting in enhanced PLQY of the PNCs. In the fabrication of blue PNCs LEDs, this approach yielded a comparable efficiency with an EQE of 5.37 % at 469 nm, demonstrating the robustness of our method for efficient blue perovskite LEDs. Furthermore, the peak wavelengths of benzoyl halide-treated PNCs LEDs remained stable during operation, whereas those of pristine PNC LEDs exhibited peak shifts. We believe that our novel approach can be universally applied to various types of perovskites, reducing bulk vacancies. This advancement will be a significant breakthrough for the performance enhancement of blue perovskite LEDs in the future.

Surficial Homogenic Effect Enables Highly Stable Deep-Blue Perovskite Light-Emitting Diodes.

The device performance of deep-blue perovskite light-emitting diodes (PeLEDs) is primarily constrained by low external quantum efficiency (EQE) especially poor operational stability. Herein, we develop a facile strategy to improve deep-blue emission through rational interface engineering. We innovatively reported the novel electron transport material, 4,6-Tris(4-(diphenylphosphoryl)phenyl)-1,3,5-triazine (P-POT2T), and utilized a sequential wet-dry deposition method to form the homogenic gradient interface between electron transport layer (ETL) and perovskite surface. Unlike previous reports that achieved carrier injection balance by inserting new interlayers, our strategy not only passivated uncoordinated Pb2+ in the perovskite via P=O functional groups but also reduced interfacial carrier recombination without introducing new interfaces. Additionally, this strategy enhanced the interface contact between the perovskite and ETL, significantly boosting device stability. Consequently, the fabricated deep-blue PeLEDs delivered an EQE exceeding 5 % (@ 460 nm) with an exceptional halftime extended to 31.3 minutes. This straightforward approach offers a new strategy to realize highly efficient especially stable PeLEDs.

Surficial Homogenic Effect Enables Highly Stable Deep‐Blue Perovskite Light‐Emitting Diodes

AbstractThe device performance of deep‐blue perovskite light‐emitting diodes (PeLEDs) is primarily constrained by low external quantum efficiency (EQE) especially poor operational stability. Herein, we develop a facile strategy to improve deep‐blue emission through rational interface engineering. We innovatively reported the novel electron transport material, 4,6‐Tris(4‐(diphenylphosphoryl)phenyl)‐1,3,5‐triazine (P‐POT2T), and utilized a sequential wet‐dry deposition method to form the homogenic gradient interface between electron transport layer (ETL) and perovskite surface. Unlike previous reports that achieved carrier injection balance by inserting new interlayers, our strategy not only passivated uncoordinated Pb2+ in the perovskite via P=O functional groups but also reduced interfacial carrier recombination without introducing new interfaces. Additionally, this strategy enhanced the interface contact between the perovskite and ETL, significantly boosting device stability. Consequently, the fabricated deep‐blue PeLEDs delivered an EQE exceeding 5 % (@ 460 nm) with an exceptional halftime extended to 31.3 minutes. This straightforward approach offers a new strategy to realize highly efficient especially stable PeLEDs.

Doping Up the Light: A Review of A/B-Site Doping in Metal Halide Perovskite Nanocrystals for Next-Generation LEDs.

All-inorganic metal halide perovskite nanocrystals (PeNCs) show great potential for the next generation of perovskite light-emitting diodes (PeLEDs). However, trap-assisted recombination negatively impacts the optoelectronic properties of PeNCs and prevents their widespread adoption for commercial exploitation. To mitigate trap-assisted recombination and further enhance the external quantum efficiency of PeLEDs, A/B-site doping has been widely investigated to tune the bandgap of PeNCs. The bandgap of PeNCs is adjustable within a small range (no more than 0.1 eV) by A-site cation doping, resulting in changes in the bond length of Pb-X and the angle of [PbX6]4. Nevertheless, B-site doping of PeNCs has a more significant impact on the bandgap level through modification of surface defect states. In this perspective, we delve into the synthesis of PeNCs with A/B-site doping and their impacts on the structural and optoelectronic properties, as well as their impacts on the performance of subsequent PeLEDs. Furthermore, we explore the A-site and B-site doping mechanisms and the impact of device architecture on doped PeNCs to maximize the performance and stability of PeLEDs. This work presents a comprehensive overview of the studies on A-site and B-site doping in PeNCs and approaches to unlock their full potential in the next generation of LEDs.

Elevating Charge Transport Layer for Stable Perovskite Light-Emitting Diodes.

Ion migration is a major factor affecting the long term stability of perovskite light-emitting diodes (LEDs), which limits their commercialization potential. The accumulation of excess halide ions at the grain boundaries of perovskite films is a primary cause of ion migration in these devices. Here, it is demonstrated that the channels of ion migrations can be effectively impeded by elevating the hole transport layer between the perovskite grain boundaries, resulting in highly stable perovskite LEDs. The unique structure is achieved by reducing the wettability of the perovskites, which prevents infiltration of the upper hole-transporting layer into the spaces of perovskite grain boundaries. Consequently, nanosized gaps are formed between the excess halide ions and the hole transport layer, effectively suppressing ion migration. With this structure, perovskite LEDs with operational half-lifetimes of 256 and 1774 h under current densities of 100 and 20mAcm-2 respectively are achieved. These lifetimes surpass those of organic LEDs at high brightness. It is further found that this approach can be extended to various perovskite LEDs, showing great promise for promoting perovskite LEDs toward commercial applications.

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

Metal Halide Perovskites: Promising Materials for Light-Emitting Diodes

Metal halide perovskites have shown excellent optoelectronic properties, including high photoluminescence quantum yield, tunable emission wavelengths, narrow full-width at half-maximums and a low-cost, solution-processed fabrication, which make it exhibit great potential as emission-layer materials of light-emitting diodes. With the joint efforts of researchers from different disciplines, there has been a significant progress in the improvement in the external quantum efficiency (EQE) and stability of perovskite light-emitting diodes (PeLEDs) in recent years, especially in green PeLEDs with EQEs over 30%. However, their operational stability lags behind other commercial organic and chalcogenide quantum dot emitters, limiting their practical application. In this review, we first introduce the basic device structure of PeLEDs, as well as the factors influencing the EQE and stability of PeLEDs. Secondly, the development of lead-based and lead-free PeLEDs are summarized systematically. Thirdly, challenges of PeLEDs are discussed in detail, including low the EQE of blue PeLEDs, poor device stability and EQE roll-off. Finally, some suggestions and perspectives for future research directions for PeLEDs are proposed.

Perovskite nanocrystals passivated by aromatic phosphonic acid for high-performance light-emitting diodes

Here the authors presented BPA-passivated FAPbBr3 NCs. The presence of –PO groups in the BPA plays a critical role in preventing superoxide formation, resulting in high-performance LEDs with an efficiency of 12.9% and a luminance of 29 280 cd m−2.

Low-dimensional nanomaterial-enabled efficient and stable perovskite light-emitting diodes: recent progress and challenges

This article reviews the research progress and challenges of multi-functional low-dimensional nanomaterials in advanced perovskite light-emitting diodes.

Advances and future perspectives in polycrystalline halide perovskite light-emitting diodes

Metal halide perovskites (MHPs) have emerged as a highly promising candidate for next-generation light-emitting materials due to their exceptional optoelectronic properties. These properties include superior color purity, high photoluminescence quantum efficiency (PLQY), and the facile tunability of bandgap through compositional and dimensional control. Particularly, polycrystalline perovskites have been introduced as the first perovskite light-emitting diodes (PeLEDs) with superior charge mobility. However, the development of efficient and stable PeLEDs, crucial for commercialization, has proven to be a significant challenge due to the low exciton binding energy (E b) and inherent defects. Nevertheless, recent achievements have demonstrated polycrystalline PeLEDs with an external quantum efficiency (EQE) surpassing 28% and a half-lifetime (T 50) exceeding 30,000 h. In this review, we present the progress of polycrystalline PeLEDs with improved efficiency (PLQY, EQE) and stability by focusing on grain size regulation, defect passivation, and dimensional control. This review offers promising strategies for realizing polycrystalline perovskite material as a light emitter, highlights limitations and provides future perspectives for advancing PeLEDs.

Iodotrimethylsilane as a Reactive Ligand for Surface Etching and Passivation of Perovskite Nanocrystals toward Efficient Pure-red to Deep-red LEDs.

Resurfacing perovskite nanocrystals (NCs) with tight-binding and conductive ligands to resolve the dynamic ligands - surface interaction is the fundamental issue for their applications in perovskite light-emitting diodes (PeLEDs). Although various types of surface ligands have been proposed, these ligands either exhibit weak Lewis acid/based interactions or need high polar solvents for dissolution and passivation, resulting in a compromise in the efficiency and stability of PeLEDs. Herein, we report a chemically reactive agent (Iodotrimethylsilane, TMIS) to address the trade-off among conductivity, solubility and passivation using all-inorganic CsPbI3 NCs. The liquid TMIS ensures good solubility in non-polar solvents and reacts with oleate ligands and produces in-situ HI for surface etching and passivation, enabling strong-binding ligands on the NCs surface. We report, as a result, red PeLEDs with an external quantum efficiency (EQE) of ~23%, which is 11.2-fold higher than the control, and is among the highest CsPbI3 PeLEDs. We further demonstrate the university of this ligand strategy in the pure bromide system (CsPbBr3), and report EQE of ~20% at 640, 652, and 664 nm. This represents the first demonstration of ligand strategy that applies to different systems and works effectively in red PeLEDs spanning emission from pure-red to deep-red.

Iodotrimethylsilane as a Reactive Ligand for Surface Etching and Passivation of Perovskite Nanocrystals toward Efficient Pure‐red to Deep‐red LEDs

AbstractResurfacing perovskite nanocrystals (NCs) with tight‐binding and conductive ligands to resolve the dynamic ligands—surface interaction is the fundamental issue for their applications in perovskite light‐emitting diodes (PeLEDs). Although various types of surface ligands have been proposed, these ligands either exhibit weak Lewis acid/base interactions or need high polar solvents for dissolution and passivation, resulting in a compromise in the efficiency and stability of PeLEDs. Herein, we report a chemically reactive agent (Iodotrimethylsilane, TMIS) to address the trade‐off among conductivity, solubility and passivation using all‐inorganic CsPbI3 NCs. The liquid TMIS ensures good solubility in non‐polar solvents and reacts with oleate ligands and produces in situ HI for surface etching and passivation, enabling strong‐binding ligands on the NCs surface. We report, as a result, red PeLEDs with an external quantum efficiency (EQE) of ≈23 %, which is 11.2‐fold higher than the control, and is among the highest CsPbI3 PeLEDs. We further demonstrate the universality of this ligand strategy in the pure bromide system (CsPbBr3), and report EQE of ≈20 % at 640, 652, and 664 nm. This represents the first demonstration of a chemically reactive ligand strategy that applies to different systems and works effectively in red PeLEDs spanning emission from pure‐red to deep‐red.

Bright and stable perovskite light-emitting diodes in the near-infrared range.

Perovskite light-emitting diodes (LEDs) have attracted broad attention due to their rapidly increasing external quantum efficiencies (EQEs)1-15. However, most high EQEs of perovskite LEDs are reported at low current densities (<1 mA cm-2) and low brightness. Decrease in efficiency and rapid degradation at high brightness inhibit their practical applications. Here, we demonstrate perovskite LEDs with exceptional performance at high brightness, achieved by the introduction of a multifunctional molecule that simultaneously removes non-radiative regions in the perovskite films and suppresses luminescence quenching of perovskites at the interface with charge-transport layers. The resulting LEDs emit near-infrared light at 800 nm, show a peak EQE of 23.8% at 33 mA cm-2 and retain EQEs more than 10% at high current densities of up to 1,000 mA cm-2. In pulsed operation, they retain EQE of 16% at an ultrahigh current density of 4,000 mA cm-2, along with a high radiance of more than 3,200 W s-1 m-2. Notably, an operational half-lifetime of 32 h at an initial radiance of 107 W s-1 m-2 has been achieved, representing the best stability for perovskite LEDs having EQEs exceeding 20% at high brightness levels. The demonstration of efficient and stable perovskite LEDs at high brightness is an important step towards commercialization and opens up new opportunities beyond conventional LED technologies, such as perovskite electrically pumped lasers.

A Mixed Organic-Inorganic Interlayer With Tunable Electrical Properties Enabling Stable and Efficient Perovskite Light-Emitting Diodes

The operational stability of perovskite light-emitting diodes (PeLEDs) is subjected to undesired Joule heating induced by the charge imbalance and the current leakage. The hole injection efficiency is inferior to that of electrons in the electron-dominated PeLEDs, owing to the low hole mobility of hole transport materials and a relatively large hole injection barrier. Herein, we inserted a mixed interlayer of 4,7-diphenyl-1,10-phenanthroline and cesium carbonate (Bphen:Cs2CO3) (~10 nm) between the electron transport layer (ETL) TPBi and the metal cathode to improve the charge imbalance by optimizing the electron injection and suppressing the current leakage. Compared to TPBi, the Bphen interlayer builds a larger electron injection barrier from the cathode to perovskite layer owing to its shallower lowest unoccupied molecular orbital (LUMO), leading to inefficient electron injection. The Cs2CO3, an n-type dopant, was co-evaporated with Bphen to increase the conductivity and thus balance the electron and hole transport. The resultant quasi-2D PeLED achieves an external quantum efficiency of 17.62% and an operational lifetime of over 1900 min at an initial luminance of 100 cd <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$\text{m}^{-{2}}$ </tex-math></inline-formula> .

Manipulating Crystallization Dynamics for Efficient and Spectrally Stable Blue Perovskite Light‐Emitting Diodes

AbstractReduced‐dimensional perovskite light‐emitting diodes (PeLEDs) have shown great potential in solution‐processed high‐definition displays. However, the inferior electroluminescent (EL) performance of blue PeLEDs has become a huge challenge for their commercialization. The inefficient domain control [number of PbX6− layers (n)] and deleterious phase segregation make the blue PeLEDs suffer from low EL efficiency and poor spectral stability. Here, a rational strategy for perovskite crystallization control by adjusting the precursor concentration is proposed for improving phase distribution and suppressing ion migration in reduced‐dimensional mixed‐halide blue perovskite films. Based on this method, efficient sky‐blue PeLEDs exhibit a maximum external quantum efficiency (EQE) of 8.5% with stable EL spectra at 482 nm. Additionally, spectrally stable pure‐blue PeLEDs at 474 and 468 nm are further obtained with maximum EQEs of 4.0% and 2.4%, respectively. These findings may provide an alternative scheme for manipulating perovskite crystallization dynamics toward efficient and stable PeLEDs.

Degradation mechanisms of perovskite light-emitting diodes under electrical bias

Abstract Metal-halide perovskite light-emitting diodes (PeLEDs) are considered as new-generation highly efficient luminescent materials for application in displays and solid-state lighting. Since the first successful demonstration of PeLEDs in 2014, the research on the development of efficient PeLEDs has progressed significantly. Although the device efficiency has significantly improved over a short period of time, their overall performance has not yet reached the levels of mature technologies for practical applications. Various degradation processes are the major impediment to improving the performance and stability of PeLED devices. In this review, we discuss various analysis techniques that are necessary to gain insights into the effects of various degradation mechanisms on the performance and stability of PeLEDs. Based on the causes and effects of external and internal factors, the degradation processes and associated mechanisms are examined in terms of critical physical and chemical parameters. Further, according to the progress of the current research, the challenges faced in studying degradation mechanisms are also elucidated. Given the universality of the degradation behavior, an in-depth understanding of the device degradation may promote the development of optimization strategies and further improve the performance and stability of PeLEDs.

Ultra-bright, efficient and stable perovskite light-emitting diodes.

Metal halide perovskites are attracting a lot of attention as next-generation light-emitting materials owing to their excellent emission properties, with narrow band emission1-4. However, perovskite light-emitting diodes (PeLEDs), irrespective of their material type (polycrystals or nanocrystals), have not realized high luminance, high efficiency and long lifetime simultaneously, as they are influenced by intrinsic limitations related to the trade-off of properties between charge transport and confinement in each type of perovskite material5-8. Here, we report an ultra-bright, efficient and stable PeLED made of core/shell perovskite nanocrystals with a size of approximately 10 nm, obtained using a simple in situ reaction of benzylphosphonic acid (BPA) additive with three-dimensional (3D) polycrystalline perovskite films, without separate synthesis processes. During the reaction, large 3D crystals are split into nanocrystals and the BPA surrounds the nanocrystals, achieving strong carrier confinement. The BPA shell passivates the undercoordinated lead atoms by forming covalent bonds, and thereby greatly reduces the trap density while maintaining good charge-transport properties for the 3D perovskites. We demonstrate simultaneously efficient, bright and stable PeLEDs that have a maximum brightness of approximately 470,000 cd m-2, maximum external quantum efficiency of 28.9% (average = 25.2 ± 1.6% over 40 devices), maximum current efficiency of 151 cd A-1 and half-lifetime of 520 h at 1,000 cd m-2 (estimated half-lifetime >30,000 h at 100 cd m-2). Our work sheds light on the possibility that PeLEDs can be commercialized in the future display industry.

Impacts of the Lattice Strain on Perovskite Light‐Emitting Diodes

AbstractThe development of perovskite light‐emitting diodes (PeLEDs) with both high efficiency and excellent stability remains challenging. Herein, a strong correlation between the lattice strain in perovskite films and the stability of resulting PeLEDs is revealed. Based on high‐efficiency PeLEDs, the device lifetime is optimized by rationally tailoring the lattice strain in perovskite films. A PeLED with a high peak external quantum efficiency of 18.2% and a long lifetime of 151 h (T70, under a current density of 20 mA cm−2) is realized with a minimized lattice strain in the perovskite film. In addition, an increase in the lattice strain is found during the long‐time device stability test, indicating that the degradation of the local perovskite lattice structure could be one of the degradation mechanisms for long‐term stable PeLEDs.

Strategies to Improve the Stability of Perovskite Light-Emitting Diodes: Progress and Perspective.

Perovskite light-emitting diodes (PeLEDs) featuring excellent electroluminescent (EL) characteristics and facile production have been emerging as promising candidates for next-generation high-definition displays. In recent years, tremendous advances have been achieved in the EL efficiency of PeLEDs. However, their poor operational stability impedes practical applications. Particularly, the severe spectral instability of pure-blue and pure-red PeLEDs lags far behind the requirements of commercial displays. In this Perspective, the critical factors related to device degradation are first summarized, including perovskite crystal defects, unbalanced charge injection, Auger recombination, and Joule heating. Then, the recent progress in improving the operational and spectral stabilities is reviewed in categories. Considering the present achievements, we provide potential research directions for further development of stable PeLEDs.