Strategies Toward Efficient Blue Perovskite Light-Emitting Diodes

Substantial progress has been made in blue perovskite light-emitting diodes (PeLEDs). In this review, the strategies for high-performance blue PeLEDs are described, and the main focus is on the optimization of the optical and electrical properties of perovskites. In detail, the fundamental device working principles are first elucidated, followed by a systematical discussion of the key issues for achieving high-quality perovskite nanocrystals (NCs) and quasi-2D perovskites. These involve ligand optimization and metal doping in enhancing the carrier transport and reducing the traps of perovskite NCs, as well as the perovskite phase modulation and defect passivation in improving energy transfer and emission efficiency of quasi-2D perovskites. The strategies for efficient 3D mixed-halide perovskite and lead-free perovskite blue LEDs are then briefly introduced. After that, other strategies, including effective charge transport layer, efficient perovskite emission system, and effective device architecture for high light outcoupling efficiency, are further discussed to boost the blue PeLED performances. Meanwhile, the testing standard of blue PeLED lifetime is suggested to enable the direct comparisons of the device operational stability. Finally, challenges and future directions for blue PeLEDs are addressed.     

Manipulating Ionic Behavior with Bifunctional Additives for Efficient Sky-Blue Perovskite Light-Emitting Diodes

Perovskite Light-emitting diodes (PeLEDs) have emerged as a promising technique for future high-definition displays due to their outstanding electroluminescent characters. However, the development of blue PeLEDs toward practical applications is seriously hindered by their inferior performance, which mainly arises from the detrimental halide ionic behavior and thus severe nonradiative recombination in mixed-halide blue perovskite materials. Herein, efficient sky-blue PeLEDs featuring spectrally stable emission at 483 nm are realized by employing bifunctional passivators of Lewis-base benzoic acid anions and alkali metal cations to simultaneously passivate the under-coordinated lead atoms and suppress halide ion migration. A decent external quantum efficiency (EQE) of 16.58% and a maximum EQE of 18.65% are achieved, which is further boosted to 28.82% through the optical outcoupling enhancement. This work demonstrates unique insight into the generality and individuality of this category of benzoates and puts forward a feasible guidance in choosing appropriate additives for efficient perovskite materials.     

Efficient and Stable Perovskite White Light-Emitting Diodes for Backlit Display

High-quality backlit display puts forward urgent demand for color-converting materials. Recently, metal halide perovskites (MHPs) with full spectral tunability, high photoluminescence quantum yields (PLQYs), and high color purity have found potential application in wide-color-gamut display. Regrettably, naked MHPs suffer from long-term instable issue and cannot pass harsh stability tests. Herein, amorphous-glass-protected green/red CsPbX₃ quantum dots (QDs) are prepared by elaborately optimizing glass structure, perovskite concentration, and in situ crystallization. PLQYs of green CsPbBr₃@glass and red CsPbBr_1.5I_1.5@glass reach 94% and 78%, respectively, which are the highest ones of CsPbX₃@glass composites reported so far and comparable to colloidal counterparts. Benefited from complete isolation of QDs from external environment by glass network, CsPbX₃@glass can endure harsh commercial standard aging tests of 85 °C/85%RH and blue-light-irradiation, which are applied to construct white light-emitting diodes (wLEDs) with high external quantum efficiency of 13.8% and ultra-high luminance of 500 000 cd m⁻². Accordingly, the perovskite wLED arrays-based backlit unit and a prototype display device are designed for the first time, showing more vivid and wide-color-gamut feature benefited from narrowband emissions of CsPbX₃ QDs. This work highlights practical application of CsPbX₃@glass composite as an efficient and stable light color converter in backlit display.     

Interfacial Potassium-Guided Grain Growth for Efficient Deep-Blue Perovskite Light-Emitting Diodes

Perovskite light-emitting diodes (PeLEDs) are emerging candidates for the applications of solution-processed full-color displays. However, the device performance of deep-blue PeLED still lags far behind that of their red and green counterparts, which is largely limited by low external quantum efficiency (EQE) and poor operational stability. Here, a facile and reliable crystallization strategy for perovskite grains is proposed, with improved deep-blue emission through rational interfacial engineering. By modifying the substrate with potassium cation (K⁺) as the supplier of heterogeneous nucleation seeds, the interfacial K⁺-guided grain growth is realized for well-packed perovskite assemblies with high surface coverage and the controlled crystal orientation, leading to the enhanced radiative recombination and hole-transport capabilities. Synergistical boost in device performance is achieved for deep-blue PeLEDs emitting at 469 nm with a peak EQE of 4.14%, a maximum luminance of 451 cd m^–2, and spectrally stable color coordinates of (0.125, 0.076) that matches well with the National Television System Committee (NTSC) standard blue.     

Color-Stable Deep-Blue Perovskite Light-Emitting Diodes Based on Organotrichlorosilane Post-Treatment

Recent studies of sky-blue perovskite light-emitting diodes (PeLEDs) have extensively promoted optimal device design to achieve an external quantum efficiency (EQE) above 12%. However, the development of thin-film deep-blue PeLEDs lags dramatically behind, especially with regards to meeting the latest Rec. 2020 standard. A trichloro(3,3,3-trifluoropropyl) silane post-treatment that drives the emission of perovskite into the deep-blue region, ranging from 440 to 460 nm, which meets the Rec. 2020 standard, is proposed. The chlorine ions released from the organotrichlorosilane molecules during their polycondensation reaction provide an addition halide source to fine tune the composition of the mixed halide perovskite films, leading to increase of bandgap and deep-blue emission. In addition, hydrogen bonds between the hydroxy groups of silane molecules and halide anions in perovskite can suppress ion migration for improving emission stability. As a result, an optimal PeLED is developed with deep-blue emission at 458 nm and excellent color stability, which yields an EQE and luminance of 1.1% and 130 cd m⁻², respectively, representing a state-of-the-art result for thin-film PeLEDs in this emission region. This work paves the way to achieve high-performance deep-blue PeLEDs with stable emissions to meet the demand for potential applications such as full-color display.     

Minimizing Optical Energy Losses for Long-Lifetime Perovskite Light-Emitting Diodes

Regardless of the rapid advance on perovskite light-emitting diodes (PeLEDs), the lack of long-term operational stability hinders the practicality of this technology. Particularly, thermal management is indispensable to control the Joule heating induced by charge transport and parasitic re-absorption of internally confined photons. Herein, a synergetic device architecture is proposed for minimizing the optical energy losses in PeLEDs toward high efficiency and long lifetime. By adopting a carefully modified perovskite emitter in combination with an improved light outcoupling structure, red PeLEDs emitting at 666 nm achieve a peak external quantum efficiency of 21.2% and an operational half-lifetime of 4806.7 h for an initial luminance of 100 cd m^-2. The enhanced light extraction from trapped modes can efficiently reduce the driving current and suppress optical energy losses in PeLEDs, which in turn ameliorate the heat-induced device degradation during operation. This work paves the way toward high-performance PeLEDs for display and lighting applications in the future.     

Suppressing Ion Migration of Mixed-Halide Perovskite Quantum Dots for High Efficiency Pure-Red Light-Emitting Diodes

Perovskite-based light-emitting diodes (PeLEDs) with a mixed halide composition can be used to obtain the “pure red” emission, i.e., in the 620–650 nm range, required for high-definition displays. However, fast halide ion migration induces phase separation in these materials under electric fields, resulting in poor spectral stability and low efficiency. Herein, a method for producing mixed halide CsPbI_3-xBr_x quantum dots (QDs) is reported in which ion migration is suppressed. The mixed halide composition is first achieved by anion exchange between CsPbI₃ QDs and hydrobromic acid (HBr), during that the bromine ions efficiently passivate the iodine vacancies of the QDs. The original oleic acid ligands are then exchanged for 1-dodecanethiol (1-DT), which suppresses halide ion migration via the strong binding of the sulfhydryl group with the QD surface. PeLEDs based on these QDs exhibit a pure-red electroluminescence (EL) peak at 637 nm, a maximum external quantum efficiency (EQE) of 21.8% with an average value of 20.4%, a peak luminance of 2653 cd m⁻², and low EQE decease with increasing luminance. The EL spectrum of these devices is stable even at 6.7 V and they have an EQE half-life of 70 min at an initial luminance of 150 cd m⁻².     

Efficient All-Perovskite White Light-Emitting Diodes Made of In Situ Grown Perovskite-Mesoporous Silica Nanocomposites

Metal halide perovskite quantum dots (QDs) have emerged as potential materials for high brightness, wide color gamut, and cost-effective backlight emission due to their high photoluminescence quantum yields, narrow emission linewidths, and tunable bandgaps. Herein, CsPbX₃/SBA-15 nanocomposites are prepared with outstanding optical properties and high stability through an in situ growth strategy using mesoporous silica particles. According to finite-difference time-domain simulations, the mesoporous structure provides a strong waveguide effect on perovskite QDs and the uniform dispersion suppresses reabsorption losses, improving the overall photoconversion efficiency of perovskite QDs. The as-fabricated perovskite monochromatic light-emitting diode (LED) has a maximum luminous efficiency of 183 lm W⁻¹, which is the highest for monochromatic perovskite LEDs reported to date. A further benefit of this work is that the white devices, which combine the green and red perovskite nanocomposites with commercial blue LED, exhibit a high luminous efficiency of 116 lm W⁻¹ and a wide color gamut (125% for NTSC and 94% for Rec. 2020) with coordinates of (0.33,0.31).     

Domain Controlling by Compound Additive toward Highly Efficient Quasi-2D Perovskite Light-Emitting Diodes

Quasi-2D perovskites with enlarged exciton binding energy and tunable bandgap are appealing for application in perovskite light-emitting diodes (PeLEDs). However, wide n domains distribution is commonly formed in solution-processed quasi-2D perovskite films due to the uncontrollable crystallization behavior, which leads to low device performance. Here, the crystallization process is successfully regulated to narrow the n domains distribution by introducing compound additive of ZrO₂ nanoparticles (NPs) and Cryptand complexant. ZrO₂ NPs can avoid the segregation of organic large and small cations by strengthening the solvent extraction capacity of antisolvent, while Cryptand offsets the poor solubility of PbBr₂ by forming an intermediate state to slow down the crystallization of high-n domains. Consequently, both high photoluminescence quantum yields over 90% and a high external quantum efficiency of 21.2% are obtained in the optimized green quasi-2D PeLEDs. Moreover, the lifetime extends about four times compared with control devices. The strategy of domain controlling by compound additive provides a powerful way to develop high-performance quasi-2D perovskite optoelectrical devices.     

Stable and Bright Pyridine Manganese Halides for Efficient White Light-Emitting Diodes

Highly efficient lead halide perovskites with tunable emission performance have become new candidate materials for light-emitting devices and displays; however, the toxicity of lead and instability of halide perovskites greatly limits their application. Herein, rapid and large-scale synthesis of highly emissive organic–inorganic manganese halide perovskites, (C₅H₆N)₂MnBr₄ and C₅H₆NMnCl₃, are presented by a one-pot solution-based method, of which (C₅H₆N)₂MnBr₄ displays a high absolute photoluminescence quantum yield (95%) in the solid-state. The developed (C₅H₆N)₂MnBr₄ perovskite noticeably exhibits high stability. Therefore both as-synthesized green and red emissive manganese-based phosphors with superior optical properties are used to fabricate blue light pumped white light-emitting diodes (WLEDs), displaying excellent quality white light with a high color rendering index value of 91 and a correlated color temperature of 5331 K. This study not only presents the robust large-scale production synthetic approach for organic–inorganic manganese halide perovskites, but also facilitates the development of high-performance phosphors for future lighting and display technologies.     

Holy Water: Photo-Brightening in Quasi-2D Perovskite Films under Ambient Enables Highly Performing Light-Emitting Diodes

Quasi-2D perovskites provide new opportunities for lighting and display applications due to their high radiative recombination and excellent stability. However, seldom attention has been placed on their self-stability/working operation under ambient storage. Herein, quasi-2D perovskites/Polyethylene oxide (PEO) films are studied, showing an unforeseen photo-brightening effect under ambient storage (i.e., an increase of the photoluminescence quantum yield from 55% to 74% after 100 days). In stark contrast, those stored under a dark/inert atmosphere show a significant decrease down to 38%. This counterintuitive phenomenon responds to the increasing radiative recombination rate caused by the passivation of the surface Br vacancies in the presence of physically adsorbed water molecules, as corroborated by in situ/ex situ X-ray photoelectron spectroscopy and density functional theory calculations. Capitalizing on this surprising effect, stable light-emitting diodes (LEDs) using quasi-2D perovskites/PEO color filters are fabricated, realizing high stabilities of ≈400 h@10 mA under operating ambient conditions, representing a 20-fold enhancement compared to LEDs with 3D counter partners. Hence, this study reveals a unique insight into the impact of water passivation on the optical/structural properties of quasi-2D perovskite films, broadening their applications under operating ambient conditions.     

Efficient and Spectrally Stable Blue Perovskite Light‐Emitting Diodes Based on Potassium Passivated Nanocrystals

Metal halide perovskites have aroused tremendous interest in the past several years for their promising applications in display and lighting. However, the development of blue perovskite light‐emitting diodes (PeLEDs) still lags far behind that of their green and red cousins due to the difficulty in obtaining high‐quality blue perovskite emissive layers. In this study, a simple approach is conceived to improve the emission and electrical properties of blue perovskites. By introducing an alkali metal ion to occupy some sites of peripheral suspended organic ligands, the nonradiative recombination is suppressed, and, consequently, blue CsPb(Br/Cl)₃ nanocrystals with a high photoluminescence quantum efficiency of 38.4% are obtained. The introduced K⁺ acts as a new type of metal ligand, which not only suppresses nonradiative pathways but also improves the charge carrier transport of the perovskite nanocrystals. With further engineering of the device structure to balance the charge injection rate, a spectrally stable and efficient blue PeLED with a maximum external quantum efficiency of 1.96% at the emission peak of 477 nm is fabricated.     

High-Performance Perovskite-Based Blue Light-Emitting Diodes with Operational Stability by Using Organic Ammonium Cations as Passivating Agents

Blue emissive perovskites can be prepared by incorporating chlorine into bromine-based perovskites to tune their bandgap. However, mixed-halide perovskites exhibit intrinsic phase instability, particularly under electrical potential, owing to halide migration. To achieve high-performance blue perovskite-based light-emitting diodes (PeLEDs) with operational stability, organic ammonium cations are used for passivating the anionic defects of the CsPbBr₂Cl film. Diphenylpropylammonium chloride (DPPACl), used as a passivating agent, successfully prevents the spectral instability of blue PeLEDs by passivating the Cl⁻ vacancies. Consequently, the blue PeLED prepared with this passivating agent delivers excellent device performance with a maximum external quantum efficiency of 3.03%. Moreover, upon tuning the DPPACl concentration, the PeLED emits stably in the deep-blue spectral region (464 nm) with a half-life time of 420 s. Thus, the use of organic ammonium cation as a passivating agent is an effective strategy for developing high-performance blue PeLEDs with operational stability.     

Emission Wavelength Tuning via Competing Lattice Expansion and Octahedral Tilting for Efficient Red Perovskite Light-Emitting Diodes

The band-edge electronic structure of lead halide perovskites (ABX₃) is composed of the orbitals of B and X components and can be tuned through the composition and structure of the BX₆ octahedron. Although A-site cations do not directly contribute to near-edge states, the bandgap of 3D metal halide perovskites can be affected by A-cations through BX₆ octahedron tilting or lattice size variation. Here, as confirmed by the Rietveld refinement results of X-ray diffraction characterization, the competition between lattice expansion and octahedral tilting is identified for the first time in emission wavelength tuning when introducing a large A-site cation (C₂H₅NH₃⁺, EA⁺) into 1-naphthylmethylammonium iodide-passivated CsPbI₃ system. The former dominates spectral redshift, while the latter leads to a blueshift of emission peak, which broadens the way to tune the emission wavelength. In addition, excess cations can also passivate the perovskites, leading to a photoluminescence (PL) quantum yield as high as 61%, increased average PL lifetime of 74.7 ns, and a high radiative and non-radiative recombination ratio of 15.7. Eventually, spectral-stable deep-red perovskite light-emitting diode with a maximum external quantum efficiency of 17.5% is realized, which is one of the highest efficiencies without using any light outcoupling and anti-solvent techniques.     

Suppressing Ion Migration Enables Stable Perovskite Light‐Emitting Diodes with All‐Inorganic Strategy

Stability issue is one of the major concerns that limit emergent perovskite light‐emitting diodes (PeLEDs) techniques. Generally, ion migration is considered as the most important origin of PeLEDs degradation. In this work, an all‐inorganic device architecture, LiF/perovskite/LiF/ZnS/ZnSe, is proposed to address this imperative problem. The inorganic (Cs_1?xRb_x)_1?yK_yPbBr₃ perovskite is optimized with achieving a photoluminescence quantum yield of 67%. Depth profile analysis of X‐ray photoelectron spectroscopy indicates that the LiF/perovskite/LiF structure and the ZnS/ZnSe cascade electron transport layers significantly suppress the electric‐field‐induced ion migrations of the perovskite layers, and impede the diffusion of metallic atoms from cathode into perovskites. The as‐prepared PeLEDs display excellent shelf stability (maintaining 90% of the initial external quantum efficiency [EQE] after 264 h) and operational stability (half‐lifetime of about 255 h at an initial luminance of 120 cd m^?2). The devices also exhibit a maximum brightness of 15 6155 cd m^?2 and an EQE of 11.05%.     

High-Performance Blue Perovskite Films and Micro-Arrays for Light-Emitting Diodes with Ionic Liquid Interlayer

Metal halide perovskites have attracted considerable attention for light-emitting diode (LED) applications due to their desirable optoelectronic properties including high brightness and color purity. However, the performance of blue perovskite LEDs (PeLEDs) remains inferior to their red and green counterparts. Herein, an ionic liquid (IL), specifically 1-butyl-3-methylimidazolium tetrafluoroborate is introduced as the interlayer on the hole transport layer (HTL). This IL demonstrates a strong interaction with the perovskite emissive layer, resulting in effective defect passivation and a shallower valence band maximum. Consequently, nonradiative recombination is reduced, and hole injection is enhanced. Additionally, a soft lithography method employing a transfer process is successfully developed that enables precise micropatterning of the perovskite light-emitting layer. Through these advancements, the IL-modified PeLED exhibits pure blue emission at 470 nm with a maximum luminance of 891 cd m⁻² and an impressive maximum EQE of 8.3%. Furthermore, the micro PeLED with an IL interlayer achieves a maximum luminance of 400 cd m⁻² and a maximum EQE of 3.9%.     

Polymer-Encapsulated Halide Perovskite Color Converters to Overcome Blue Overshoot and Cyan Gap of White Light-Emitting Diodes

Currently, the most popular way to manufacture white light-emitting diodes (WLEDs) is based on blue-emitting InGaN LED chips (440–460 nm) and yellow-emitting phosphor coating (520–700 nm) to produce white light lighting. However, because conventional white WLEDs lack the uniformly distributed continuous emission spectrum compared to natural sunlight: “blue overshoot” (extra 440–460 nm blue-light can cause damage to the retina) and “cyan gap” (470–520 nm wavelength range). Here, a novel strategy to “kill two birds with one stone” is reported: using the stable and bright polymer encapsulated perovskite nanocrystals (PNCs) composite films as the cyan color converters that efficiently absorb the “blue overshoot” and effectively emit the cyan light to fill the “cyan gap”. A series of polymer-encapsulated PNC films is achieved that can reach very high photoluminescence quantum yield (PL QY) of 90–95% under 450 nm blue-light excitation. Importantly, both 370 nm UV-excited WLED and 455 nm blue-excited WLED devices are constructed that exhibit smoothly and evenly distributed white light without blue overshoot and cyan gap, which was not achieved before for blue-excited cyan-emissive materials. This study paves the way toward the application of PNC color converters in the next generation full-visible-spectrum WLED lighting that mimic the natural daylight.     

Constructing CsPbBr3 Cluster Passivated‐Triple Cation Perovskite for Highly Efficient and Operationally Stable Solar Cells

Ion migration and phase segregation, in mixed‐cation/anion perovskite materials, raises a bottleneck for its stability improvement in solar cells operation. Here, the synergetic effect of electric field and illumination on the phase segregation of Cs_0.05FA_0.80MA_0.15Pb(I_0.85Br_0.15)₃ (CsFAMA) perovskite is demonstrated. CsFAMA perovskite with a CsPbBr₃‐clusters passivated structure is realized, in which CsPbBr₃‐clusters are located at the surface/interface of CsFAMA grains. This structure is realized by introducing a CsPbBr₃ colloidal solution into the CsFAMA precursor. It is found that CsPbBr₃ passivation greatly suppresses phase segregation in CsFAMA perovskite. The resultant passivated CsFAMA also exhibits a longer photoluminescence lifetime due to reduced defect state densities, produces highly efficient TiO₂‐based planar solar cells with 20.6% power conversion efficiency and 1.195 V open‐circuit voltage. The optimized devices do not suffer from a fast burn‐in degradation and retain 90% of their initial performance at maximum power under one‐sun illumination at 25 °C (65 °C) exceeding 500 h (100 h) of continuous operation. This result represents the most stable output among CsFAMA solar cells in a planar structure with Spiro‐OMeTAD.     

Deepening Insights into Aggregation Effect of Intermolecular Charge-Transfer Aggregates for Highly Efficient Near-Infrared Non-Doped Organic Light-Emitting Diodes over 780 nm

Though urgently needed, high-efficiency near-infrared (NIR) organic light-emitting diode (OLED) is still rare due to the energy-gap law. Formation of intermolecular charge-transfer aggregates (CTA) with nonadiabatic coupling suppression can decelerate non-radiative decay rates for high-efficiency NIR-OLEDs. However, the aggregation effect of CTA is still not fully understood, which limits the rational design of CTA. Herein, two CTA molecules with a same π-framework but different terminal substituents are developed to unveil the aggregation effect. In highly ordered crystalline states, the terminal substituents substantially affect the molecular packing motifs and intermolecular charge-transfer states, thus leading to distinct photophysical properties. In comparison, in amorphous states, these two CTA demonstrate similar photophysical behaviors and properties due to their similar molecular packing and intermolecular interactions as evidenced by molecular dynamics simulations. Importantly, the formations of amorphous CTA trigger multifunction improvements such as aggregation-induced NIR emission, aggregation-induced thermally activated delayed fluorescence, self-doping and self-host features. The non-doped OLEDs demonstrate NIR emissions centered at 788 and 803 nm, and high maximum external quantum efficiencies of 2.6% and 1.5% with small efficiency roll-off, respectively. This study provides deeper insight into the aggregation effect of CTA and lays a foundation for the development of high-efficiency NIR non-doped OLEDs.     

Bright-Multicolor,Highly Efficient,and Addressable Phosphorescent Organic Light-Emitting Fibers: Toward Wearable Textile Information Displays

Fiber-based light-emitting devices, which can be directly integrated into daily clothes, have emerged as a next-generation display form factor that can provide informational hyper-connections between humans and devices. However, although various approaches have provided advanced wearability, challenges remain for visualizing information, such as high power consumption resulting from high driving voltage and low current efficiency (CE), limited brightness making information difficult to recognize, and lack of addressability for displaying information. Here, a novel fiber-based textile display that can surmount those challenges by successfully introducing phosphorescent organic light-emitting diodes (phOLEDs) based on a dip-coating method and an addressable structure on cylinder-shaped fiber is reported. The fiber phOLEDs exhibit unprecedented optoelectronic performance, including brightness, CE, and driving voltages comparable to those of conventional glass-based OLEDs. Particularly, they show the highest CE values of 16.3, 60.7, and 16.9 cd A^–1 for red, green, and blue, respectively, among results reported thus far. Also, the fiber phOLEDs with an addressable structure implementing independent pixels can be operated by the matrix-addressable scheme. Based on unique deformability which is confirmed by flexibility tests, the performance capabilities, and addressability, letter information can be successfully visualized on daily clothes, demonstrating the potential for realizing truly wearable textile displays.