Perovskite Light-emitting Diodes Research Articles

Performance-optimized and phase purity-improved high-n quasi-two-dimensional perovskite for green light-emitting diodes

Quasi-two-dimensional (quasi-2D) perovskite has the advantage of enlarging exciton binding energy and is more suitable for efficient perovskite light-emitting diodes (PeLEDs). However, the quasi-2D perovskite films deposited with solution methods are usually mixtures of multiple phases with different inorganic layer numbers (n), unfavorable to obtaining high emission efficiency. In this study, we selected formamidinium lead bromide (FAPbBr3) as the light emitter and (2-phenylethyl)ammonium cation (PEA+) as the long-chain organic spacer cation to prepare high-n (n = 9) quasi-2D perovskite films with improved phase purity. Based on the multiple cations mixed engineering, the quality of these films improved obviously by partly replacing FA+ with minute quantities of cesium cation (Cs+). The improvement focused on remarkably enhanced photoluminescence, few low-n phases, and decreased grain sizes. The green PeLED based on the performance-optimized and phase purity-improved high-n quasi-2D perovskite reached a high brightness of 28 960 cd/m2 together with a maximum current efficiency of 44.8 cd/A and a maximum external quantum efficiency of 9.99%.

Targeted elimination of tetravalent-Sn-induced defects for enhanced efficiency and stability in lead-free NIR-II perovskite LEDs.

Eco-friendly Sn-based perovskites show significant potential for high-performance second near-infrared window light-emitting diodes (900 nm - 1700 nm). Nevertheless, achieving efficient and stable Sn-based perovskite second near-infrared window light-emitting diodes remains challenging due to the propensity of Sn2+ to oxidize, resulting in detrimental Sn4+-induced defects and compromised device performance. Here, we present a targeted strategy to eliminate Sn4+-induced defects through moisture-triggered hydrolysis of tin tetrahalide, without degrading Sn2+ in the CsSnI3 film. During the moisture treatment, tin tetrahalide is selectively hydrolyzed to Sn(OH)4, which provides sustained protection. As a result, we successfully fabricate second near-infrared window light-emitting diodes emitting at 945 nm, achieving a performance breakthrough with an external quantum efficiency of 7.6% and an operational lifetime reaching 82.6 h.

Tetraoctylammonium Bromide Interlayer between NiLiOx and Perovskite for Light-Emitting Diodes.

Physical vapor deposition is a favorable technique for fabricating light-emitting diodes (LEDs) due to its scalability and reproducibility. However, the performances of LEDs fabricated via this method are worse than those prepared via solution processing owing to the generation of high defect densities. In this study, we introduce a layer of tetraoctylammonium bromide (TOABr), an interfacial-modification compound containing four long octyl chains that are symmetrically arranged around an N atom, to reduce nonradiative recombination and trap densities in CsPbBr3. We examined the impacts of adding TOABr on perovskite thin films deposited on hole injection layers made of Li-doped NiOx and poly(3,4-ethylenedioxythiophene)/polystyrenesulfonate. Our investigations reveal that TOABr addition slightly increases crystallinity, dramatically increases photoluminescence, and achieves the preferred orientation in the perovskite films. Additionally, the interfacial layer passivates defects and improves charge balance in the device, thereby enhancing performance. Consequently, perovskite LEDs with a TOABr layer exhibit a lower turn-on voltage of 3 V than their pristine counterparts, achieving a maximum luminance of 11,133 cd m-2 and an external quantum efficiency of 1.24%, whereas the pristine perovskite LEDs achieve an EQE of 0.015%. The approach proposed in this study can be used to fabricate efficient vacuum-thermal-evaporated perovskite LEDs.

Light‐Emitting Perovskite Solar Cells: Genesis to Recent Drifts

Perovskite, a star material with extraordinary opto‐electronic properties has shown promising results in both perovskite solar cells (PSCs) and perovskite light‐emitting diodes (PeLEDs). Taking advantage of the similar configuration of PSCs and PeLEDs, next generation devices with dual functionality of light‐harvesting and light‐emission can be realized. Such devices hold enormous application prospects. However, the necessary tradeoff resulted from the opposite working principles required for each mode of operation and challenges such as non‐radiative recombination loss resulted from bulk and surface defects in perovskite films and mismatched energy levels have hindered mass production. To provide a roadmap for rationally designing efficient light emitting perovskite solar cells (LEPSCs), a comprehensive review focusing on operating principle, device architecture, recent developments and limitations is required. We begin with a brief overview of the basic principles underlying the working mechanism of LEPSCs such as photon to electricity conversion and viceversa. The focus of this review then shift towards deligently combining and overviewing the important breakthroughs reported in this newly developed field such as morphology optimization, defect passivation, interface engineering, energy level alignment and dimensional control. Finally, this work concludes with discussing future challenges and providing a roadmap for rational design of efficient and stable LEPSCs.

Ultrabright and Efficient Green Perovskite Light-Emitting Diodes Enabled by Well-Crystallized Dense CsPbBr3 Nanocubes.

Perovskite light-emitting diodes (PeLEDs) are promising for next-generation high-definition displays. One of the keys to achieving high performance PeLEDs lies in how to fabricate crystalline and dense perovskite films. However, there exist challenges to directly grow well-crystallized CsPbBr3 nanocrystal thin films on transport layers due to low solubility in solvents and fast precipitation of all-inorganic CsPbBr3, and the corresponding bright, efficient, and stable green PeLEDs have rarely been reported. Herein, we report an efficient strategy to prepare well-crystallized and dense CsPbBr3 nanocubes for ultrabright and efficient green PeLEDs. We introduce sulfobetaine zwitterion as crystallization control agent and strontium fluoride nanocrystals as nucleation seeds to grow high-quality CsPbBr3 nanocube films. Eventually, the CsPbBr3 films enable green PeLEDs with a maximum luminance of 162 767 cd m-2 and a champion external quantum efficiency of 21.3% along with a narrow spectral line width of ∼14.7 nm, representing state-of-the-art performances in green PeLEDs.

Group‐VA Doped ZnO Injection Layer for Bright and Efficient Perovskite Light‐Emitting Diodes

AbstractHeteroatom doping of the ZnO electron injection layer (EIL) is widely applied to the fabrication of high‐performance quantum‐dot and perovskite light‐emitting diodes (PeLEDs), while group‐VA atomic dopant is rarely studied. Here, VA bismuth (Bi) with strong metallicity is screened as a substitution dopant to regulate the colloid size, surface terminal, and defect density of the ZnO precursor. The as‐fabricated Bi‐doped ZnO (ZnBiO) EIL shows enhanced conductivity, passivated trap states, more n‐type nature, and appropriate band alignment with FAPbI3 (FA: formamidinium), contributing to smooth injection paths with minimal transport losses. Promoted by inhibited hydroxyl terminations of ZnBiO, the FAPbI3 crystals grown into flat nanocylinder domains with higher crystallinity and area‐thickness ratio, leading to a champion PeLED efficiency of 22.3%, a high near‐infrared radiance of 684 W sr−1 m−2, and nearly an order of magnitude extended operational stability, which shows great promise of ZnBiO as the optimal EIL for various LED application scenarios beyond classical ZnMgO.

Impact of PEDOT:PSS/Ti3C2Tx composite hole transport layer on the performance of perovskite light emitting diodes

The two-dimensional transition metal carbide MXenes, often designated by Ti3C2Tx, have garnered significant interest on account of their distinctive optoelectronic characteristics. In this paper, PEDOT:PSS/Ti3C2Tx composite hole transport layer (HTLs) was prepared by adding the MXenes material Ti3C2Tx into PEDOT:PSS, and quasi-two-dimensional perovskite light-emitting diodes (PeLEDs) were fabricated and investigated. While the addition concentration of Ti3C2Tx was 0.25 mg/mL, the optimal device shows the maximum luminance of 6250 cd/m2, and the current efficiency of 6.17 cd/A, which is 133 % and 112 % higher than the reference device without Ti3C2Tx, respectively. It is indicated that the additive incorporation of Ti3C2Tx in PEDOT:PSS can improve the efficiency of hole injection and conductivity of hole transport layer, and passivate the defects of perovskite film, thus enhancing the optoelectronic performance of PeLEDs. The findings of this study indicate that the PEDOT:PSS/Ti3C2Tx composite HTLs has considerable potential for application in PeLEDs.

Managing Edge States in Reduced-Dimensional Perovskites for Highly Efficient Deep-Blue LEDs.

Pure-halide reduced-dimensional perovskites, featuring large exciton binding energy and tunable bandgap, show great potential for high-efficiency deep-blue perovskite light-emitting diodes (PeLEDs). However, their efficiency, particularly in the low n-value phase domain ("n" represents the number of octahedral sheets), lags behind analogous perovskite emitters. Herein, it is demonstrated that the vibration of edge-dangling octahedra in the low n-value phase activates notorious exciton-phonon (EP) coupling, thereby deteriorating efficiency. To address this issue, an approach is reported to manage edge-state lattices by introducing tris(4-fluorophenyl) phosphine (TFP) ligands. Attributed to the large steric hindrance of TFP ligands and their strong binding affinity for edge-dangling octahedra, the edged-octahedral tilting reconstruction can effectively suppress lattice vibration and inhibit EP coupling. This strategy yields deep-blue emitting film with a spectral linewidth of 21nm and a photoluminescence quantum yield of 85% at low excitation densities. The resulting PeLEDs achieve deep-blue emission at 469nm, with a maximum luminance of 2,428cdm-2 and a maximum external quantum efficiency of 10.4%, marking them among the most efficient deep-blue PeLEDs reported. The strategy also showcases universality for higher n-value reduced-dimensional perovskites. It is believed that the observation, along with the edge-state management strategy, lays the groundwork for further advancements in reduced-dimensional perovskite optoelectronic devices.

Device physics of perovskite light-emitting diodes

Perovskite light-emitting diodes (LEDs) have emerged as a potential solution-processible technology that can offer efficient light emission with high color purity. Here, we explore the device physics of perovskite LEDs using simple analytical and drift-diffusion modeling, aiming to understand how the distribution of electric field, carrier densities, and recombination in these devices differs from those assumed in other technologies such as organic LEDs. High barriers to electron and hole extraction are responsible for the efficient recombination and lead to sharp build-up of electrons and holes close to the electron- and hole-blocking barriers, respectively. Despite the strongly varying carrier distributions, bimolecular recombination is surprisingly uniform throughout the device thickness, consistent with the assumption typically made in optical models. The current density is largely determined by injection from the metal electrodes, with a balance of electron and hole injection maintained by redistribution of electric field within the device by build-up of space charge.

Additive-Driven Enhancement of Crystallization: Strategies and Prospects for Boosting Photoluminescence Quantum Yields in Halide Perovskite Films for Light-Emitting Diodes.

Halide perovskite light-emitting diodes (PeLEDs) hold great potential for applications in displays and lighting. To enhance the external quantum efficiency (EQE) of PeLEDs, it is crucial to boost the photoluminescence quantum yield (PLQY) of the perovskite films. The use of additives has emerged as a powerful chemical strategy to control the crystallization process in solution-processed perovskite films. The different types of additives that can be used reflect the various types of chemical interactions with the perovskite materials, influencing their crystallization process in various possible ways. Understanding the relationship between these chemical interactions and their impact on the crystallization process is a key step for designing emitters with improved PLQY and devices with superior EQE. Following the logic chain of additive-perovskite interactions, impacts on crystallization, and subsequent enhancement of PLQY and EQE, this review discusses how additives play a pivotal role in influencing the crystallization process to enhance the PLQY of the perovskite films. Furthermore, this assessment addresses the open challenges and outlines future prospects for the development of PeLEDs.

Simultaneous Improvement in Blue-Light Emission and Operational Stability of Nanometer-Thick Perovskite Light-Emitting Diodes by Incorporating Multiple Organic/Inorganic Chloride Salts

Simultaneous Improvement in Blue-Light Emission and Operational Stability of Nanometer-Thick Perovskite Light-Emitting Diodes by Incorporating Multiple Organic/Inorganic Chloride Salts

Lateral Phase Heterojunction for Perovskite Microoptoelectronics.

Perovskite heterojunction engineering is the prerequisite but still a deficiency in the fabrication of micro-optoelectronic devices, where the present top-down or bottom-up techniques mainly focus on preparing the vertical heterojunction stacks. Perovskite lateral heterojunction structures generally rely on epitaxial growth, which cannot meet the demands of mass production of micro-devices. Here, a contact diffusion lithography technique is proposed to demonstrate a perovskite lateral phase heterojunction (LPH) polycrystalline film by ion-driven local phase transition. Under the guidance of thermodynamic simulations, methylamine contact and migration collectively promote in situ formation of α-phase formamidine-based perovskite patterns surrounded by δ-phase polymorphs. Spontaneous type-I heterojunction alignment between α- and δ-phases establishes energy funnels in the LPH film to facilitate carrier utilization and radiative recombination. The wide-bandgap δ-phase also serves as the coplanar isolator to achieve local anti-leakage for device integration. Based on the bright and stable LPH pattern layer, the near-infrared microscale perovskite light-emitting diode (micro-PeLED) with impressive device performance is achieved by following conventional device fabrication protocol. The proposed LPH enriches the perovskite heterojunction family, creates a new optoelectronic processing platform, and advances its versatile applications in micro-optoelectronics and photonics.

Effect of silver nanoparticles on the photostability and aging of CsPbBr3 nanocrystals

Abstract Perovskite nanocrystals may become a promising replacement for current phosphors in light-emitting diodes (LEDs) and screens, but the question of the stability of their optical properties remains open. One way to solve this problem could be to use plasmonic nanoparticles. In this work, we investigate the combination of all-inorganic perovskite nanocrystals synthesized by the hot-injection method with spherical Ag nanoparticles (mean diameter 53 nm). 3-fold enhancement of photoluminescence (PL) has been implemented in hybrid ‘silver-CsPbBr3-polymethyl methacrylate’ structures. The presence of silver nanoparticles reduces the likelihood of Auger processes and forms a possible silver bromide barrier layer which prevents photoinduced ion migration in the perovskite-polymer film. Plasmonic enhancement of PL partially presents during long-term samples storage within 75 days. This work may be useful in the creation of perovskite LEDs using remote phosphor technology.

Enhancing the emissive film quality: a new role of TADF materials for high-performance blue perovskite light-emitting diodes

Thermally activated delayed fluorescence (TADF) materials are widely used in the field of organic light-emitting diodes (OLEDs) because they can capture both singlet and triplet excitons for light emission. However, only scare attention has been paid to the application of TADF materials in perovskite LEDs (PeLEDs) and the understanding of effects of TADF materials in PeLEDs is limited. In this study, a new role of TADF materials for achieving high-quality perovskite films to enhance the performance of PeLEDs is emphasized. TADF materials are introduced into quasi-2D blue PeLEDs to assist in the crystallization of perovskites during film annealing and ensure the formation of high-quality films with reduced defects, enhancing device performance. Additionally, a step-like hole transport layer has been constructed to reduce the hole transport barrier, which can further enhance the performance of PeLEDs. The resultant blue PeLEDs exhibits an external quantum efficiency of 5.44%, which is 12.7-fold higher than that of the control device. Furthermore, a turn-on voltage of 2.6 V is achieved, which is the lowest for TADF-based blue PeLEDs. The findings may not only unlock a new role of TADF materials in blue PeLEDs, but also provide an alternative pathway to achieve high-performance PeLEDs.

Low-dimensional phase optimization and defect passivation of quasi-2D perovskite to enhance electroluminescence by introducing b-NA

The energy funnel effect holds significant potential for enhancing light-emitting diode (LED) performance in the Quasi-two-dimensional (Quasi-2D) perovskite, which feature a unique multi-quantum well structure. However, random phase distribution and defects within Quasi-2D films pose challenges, leading to inefficient energy transfer and nonradiative recombination, thereby limiting device performance. Here, sodium 2-naphthalene sulfonate (b-NA) is introduced into the Quasi-2D perovskite film to enhance its the optical and electrical properties. The strong interaction between the S = O group and Na+ in b-NA with the perovskite matrix leads to reduced grain size, facilitating agglomeration and densification. This modification decreases the proportion of the low-n phase, enhances thermal stability, and passivates surface defects. Therefore, compared to the control device, the maximum brightness and external quantum efficiency of Quasi-2D perovskite LEDs with the optimal concentration (8b-NA) more than double, and the operational lifetime (T50) of the unpackaged device extends from 70.1 min to 168.5 min.

Bottom Electrode Modification Enables Efficient and Bright Silicon-Based Top-Emission Perovskite Light-Emitting Diodes.

The integration of perovskites with mature silicon platform has emerged as a promising approach in the development of efficient on-chip light sources and high-brightness displays. However, the performance of Si-based green perovskite light-emitting diodes (PeLEDs) still falls significantly short compared to their red and near-infrared counterparts. In this study, it is revealed that the high work function Au, widely employed in Si-based top-emission PeLEDs as the reflective bottom electrode, exhibits considerably lower reflectivity in the green spectrum than in the longer wavelengths. Consequently, Ag electrode is introduced to replace Au to enhance the green light reflectivity, and the ultrathin MoO3 and self-assembled monolayers (SAMs) are sequentially deposited for surface modification. These results indicate that the MoO3 layer removes the energy barrier at Ag/polymer hole transport layer interface, enhancing the hole injection efficiency; while the SAMs firmly anchor onto the MoO3 layer, effectively preventing interfacial defect formation. Benefited from this organic/inorganic dual-layer modification strategy, Si-based green PeLEDs with an impressive peak external quantum efficiency of 18.2% and a maximum brightness of 81931 cd m-2 are successfully fabricated, on par with those of the red and near-infrared counterparts. This achievement marks an advancement in developing high-performance Si-based PeLEDs with full-spectrum output.

Surface Treatment Engineering Enables Highly Efficient Perovskite Light-Emitting Diodes with Significantly Enhanced Modulation Speed

Surface Treatment Engineering Enables Highly Efficient Perovskite Light-Emitting Diodes with Significantly Enhanced Modulation Speed

Lead-Free Perovskite Light-Emitting Diodes.

Metal halide perovskites have been identified as a promising class of materials for light-emitting applications. The development of lead-based perovskite light-emitting diodes (PeLEDs) has led to substantial improvements, with external quantum efficiencies (EQEs) now surpassing 30% and operational lifetimes comparable to those of organic LEDs (OLEDs). However, the concern over the potential toxicity of lead has motivated a search for alternative materials that are both eco-friendly and possess excellent optoelectronic properties, with lead-free perovskites emerging as a strong contender. In this review, the properties of various lead-free perovskite emitters are analyzed, with a particular emphasis on the more well-reported tin-based variants. Recent progress in enhancing device efficiencies through refined crystallization processes and the optimization of device configurations is also discussed. Additionally, the remaining challenges are examined, and propose strategies that may lead to stable device operation. Looking forward, the potential future developments for lead-free PeLEDs are considered, including the extension of spectral range, the adoption of more eco-friendly deposition techniques, and the exploration of alternative materials.

Modulation of Charge Transport Layer for Perovskite Light-Emitting Diodes.

Perovskite light-emitting diodes (Pero-LEDs) have garnered significant attention due to their exceptional emission characteristics, including narrow full width at half maximum, high color purity, and tunable emission colors. Recent efficiency and operational stability advancements have positioned Pero-LEDs as a promising next-generation display technology. Extensive research and review articles on the compositional engineering and defect passivation of perovskite layers have substantially contributed to the development of multi-color and high-efficiency Pero-LEDs. However, the crucial aspect of charge transport layer (CTL) modulation in Pero-LEDs remains relatively underexplored. CTL modulation not only impacts the charge carrier transport efficiency and injection balance but also plays a critical role in passivating the perovskite surface, blocking ion migration, enhancing perovskite crystallinity, and improving light extraction efficiency. Therefore, optimizing CTLs is pivotal for further enhancing Pero-LED performance. Herein, this review discusses the roles of CTLs in Pero-LEDs and categorizes both reported and potential CTL materials. Then, various CTL optimization strategies are presented, alongside an analysis of the selection criteria for CTLs in high-performance Pero-LEDs. Finally, a summary and outlook on the potential of CTL modulation to further advance Pero-LED performances are provided.

Gradient Hole Injection Inducing Efficient Exciton Recombination in Blue (475 nm) Perovskite QLEDs.

Perovskite quantum dots (QDs) are emerging as excellent light sources for light-emitting diodes (LEDs). However, the performance of blue perovskite QD-based LEDs (QLEDs) still lags behind that of red and green counterparts, which is hindered by blue perovskite QDs with broad bandgaps that tend to increase nonradiative recombination. Here, we designed a gradient energy for hole injection utilizing multiple hole injection layers (HTLs) combined with carbazole-based small-molecule modification to reduce the hole injection barrier between HTLs and QD layers and improve the hole injection efficiency, realizing efficient exciton recombination in blue perovskite QLEDs. Moreover, the QD film on the designed HTLs demonstrates a lower surface roughness and improved photoluminescence properties. The optimized blue CsPbCl3-xBrx QLEDs exhibit an impressive external quantum efficiency of 20.7% with an electroluminescence peak at 475 nm and a turn-on voltage of 2.6 V, representing the state-of-the-art for blue perovskite LEDs emitting in the range of 460-480 nm.