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.     

Interfacial Nucleation Seeding for Electroluminescent Manipulation in Blue Perovskite Light-Emitting Diodes

Efficient and stable blue emission of perovskite light-emitting diodes (PeLEDs) is a requisite toward their potential applications in full-color displays and solid-state lighting. Rational manipulation over the entire electroluminescence process is promising to break the efficiency limit of blue PeLEDs. Herein, a facile device architecture is proposed to achieve efficient blue PeLEDs for simultaneously reducing the energetic loss during electron-photon conversion and boosting the light outcoupling. Effective interfacial engineering is employed to manipulate the perovskite crystallization nucleation, enabling highly compact perovskite nanocrystal assemblies and suppressing the trap-induced carrier losses by means of interfacial hydrogen bonding interactions. This strategy contributes to a high external quantum efficiency (EQE) of 12.8% for blue PeLEDs emitting at 486 nm as well as improved operational stability. Moreover, blue PeLEDs reach a peak EQE of 16.8% with the incorporation of internal outcoupling structures for waveguided light, which can be further raised to 27.5% by integrating a lens-based structure for substrate-mode light. These results verify the validity of this strategy in producing efficient and stable blue PeLEDs for practical applications.     

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%.     

Air-Processed Blue Perovskite Light-Emitting Diodes Enabled by Manipulation of Adsorbed-Moisture-Dominated Crystallization Kinetics

The fabrication of blue perovskite light-emitting diodes (PeLEDs) in air conditions promises to liberate the manipulation procedures from the protection of inert atmosphere in the glovebox, which will remarkably promote the commercialization proceeding of perovskite-based optoelectronic devices in display applications. However, achieving air-processed blue PeLEDs in the interference of moisture meets great challenges in crystallization kinetics control. Herein, it is proposed that substrate-adsorbed moisture dominates the perovskite crystallization kinetics during the fabrication in air, and the limited moisture from nonhygroscopic substrate inhibits the nucleation of the large-n phase and allows the growth of the small-n phase, thus yielding blue quasi-2D perovskite films in a wide moisture range of 10–50% relative humidity. Then, air-processed blue PeLEDs are successfully achieved for the first time, showing a brightness of 968 cd m⁻², external quantum efficiency of 2.54% at stable peak emission of 483 nm, as well as an outstanding operating stability of 546 s at a peak brightness of 45 cd m⁻², which are favorably competitive with PeLEDs fabricated in the glovebox. This work provides a guideline for air-processed blue PeLEDs fabrication, which paves the way for air-processed PeLEDs in further application of commercialization display.     

白光有机电致发光器件最新研究进展

最近白光有机电致发光二极管(White organic light-emitting diode,WOLED)的研究和应用取得了长足的发展.由于WOLED本身无可比拟的优点,用于全色彩有机电致发光显示、照明光源以及液晶显示器的背光源.根据白光器件的不同结构,综述了WOLED最新研究进展,探讨了其中的优缺点,总结了WOLED最新应用成果,并提出了发展高效、稳定的白光器件的新思路.     

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.     

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.     

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).     

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.     

2D Ruddlesden–Popper Perovskite Nanoplate Based Deep‐Blue Light‐Emitting Diodes for Light Communication

Ruddlesden–Popper perovskite, (PEA)₂PbBr₄ (PEA = C₈H₉NH₃), is a steady and inexpensive material with a broad bandgap and a narrow‐band emission. These features make it a potential candidate for deep‐blue light‐emitting diodes (LEDs). However, due to the weak exciton binding energy, LEDs based on the perovskite thin films usually possess a very low external quantum efficiency (EQE) of <0.03%. Here, for the first time, the construction of high‐performance deep‐blue LEDs based on 2D (PEA)₂PbBr₄ nanoplates (NPs) is demonstrated. The as‐fabricated (PEA)₂PbBr₄ NPs film shows a deep‐blue emission at 410 nm with excellent stability under ambient conditions. Impressively, LEDs based on the (PEA)₂PbBr₄ NPs film deliver a bright deep‐blue emission with a maximum luminance of 147.6 cd m^?2 and a high EQE up to 0.31%, which represents the most efficient and brightest perovskite LEDs operating at deep‐blue wavelengths. Furthermore, the LEDs retain over 80% of their efficiencies for over 1350 min under ≈60% relative humidity. The steady and bright deep‐blue LEDs can be used as an excitation light source to realize white light emission, which shows the potential for light communication. The work provides scope for developing perovskite into efficient and deep‐blue LEDs for low‐cost light source and light communication.     

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.     

Band Edge Control of Quasi-2D Metal Halide Perovskites for Blue Light-Emitting Diodes with Enhanced Performance

Perovskite light-emitting diodes (PeLEDs) have received great attention for their potential as next-generation display technology. While remarkable progress has been achieved in green, red, and near-infrared PeLEDs with external quantum efficiencies (EQEs) exceeding 20%, obtaining high performance blue PeLEDs remains a challenge. Poor charge balance due to large charge injection barriers in blue PeLEDs has been identified as one of the major roadblocks to achieve high efficiency. Here band edge control of perovskite emitting layers for blue PeLEDs with enhanced charge balance and device performance is reported. By using organic spacer cations with different dipole moments, that is, phenethyl ammonium (PEA), methoxy phenethyl ammonium (MePEA), and 4-fluoro phenethyl ammonium (4FPEA), the band edges of quasi-2D perovskites are tuned without affecting their band gaps. Detailed characterization and computational studies have confirmed the effect of dipole moment modification to be mostly electrostatic, resulting in changes in the ionization energies of ≈0.45 eV for MePEA and ≈ −0.65 eV for 4FPEA based thin films relative to PEA-based thin films. With improved charge balance, blue PeLEDs based on MePEA quasi-2D perovskites show twofold increase of the EQE as compared to the control PEA based devices.     

Highly Efficient Blue Light-Emitting Diodes Based on Perovskite Film with Vertically Graded Bandgap and Organic Grain Boundary Passivation Shells

Metal halide perovskite materials have emerged as a promising class of semiconductors for high-performance optoelectronic applications, particularly for light-emitting diodes (LEDs), due to their high quantum efficiency, facile color tunability, narrow emission line widths, as well as cost-effectiveness. Despite the great successes on green and red perovskite LEDs (PeLEDs), the external quantum efficiency (EQE) of blue PeLEDs still lags far behind that of green and red counterparts. Here, wavelength tunable pure and deep blue PeLEDs with high EQE are presented, achieving 17.5% and 10.8% for emission wavelengths of 472 and 461 nm, respectively. The wavelength tenability and high EQE are attributed to the unique vertically graded bandgaps and grain boundary organic shells in the perovskite films. The results demonstrate a significant performance improvement in blue PeLEDs, provide a novel route to fabricate high-performance pure and deep blue PeLEDs that can match the performance of the green and red PeLEDs for future lighting and display applications.     

Synergistic Effect of Dual Ligands on Stable Blue Quasi‐2D Perovskite Light‐Emitting Diodes

Since the emergence of inorganic–organic hybrid perovskites a few years ago, there have been many promising achievements in the field of green and red perovskite light‐emitting diodes (PeLEDs). Nevertheless, the performance of blue‐light PeLEDs faces challenges. In this work, the unique synergy obtained by introducing two different ligands to successfully form quasi‐2D perovskite films, which can exhibit stable blue‐light emission, is utilized. The fabricated PeLEDs have a maximum external quantum efficiency of 2.62% and a half lifetime (T₅₀) of 8.8 min. Meanwhile, the electroluminescence spectrum with its peak located at 485 nm, demonstrates improved stability by applying different voltage bias. The finding in this work offers a new way to achieve steady blue PeLEDs with high performance.     

Perovskite Anion Exchange: A Microdynamics Model and a Polar Adsorption Strategy for Precise Control of Luminescence Color

Inorganic perovskite quantum dots (QDs) have natural advantages in the field of light-emitting diodes (LEDs) because of their high color purity and tunability in a wide range. However, when manufacturing efficiently mixed-anion perovskite QDs (CsPbBr_xI_3−x) to meet the requirements of the pure red color standard in the display field (≈630 nm), results are difficult to control accurately due to the lack of exploration of its microscopic mechanism. Here, a microdynamics model is constructed for anion exchange dominated by vacancies which revealed the key role of polar solvent in reducing the surface energy barrier of anions through first-principle calculations. Besides, a polar solvent construct in situ anion exchange channels method is proposed. Then, the precise control of anion exchange is demonstrated, and the precise regulation spectrum of the whole red-light range (600–680 nm) is achieved. Finally, various QD LEDs (QLEDs) based on these tunable QDs are fabricated and exhibit excellent photoelectric performance in the main red range (620–680 nm). Among them, the champion QLEDs, have peak external quantum efficiency (EQE) of 16.3% at 633 nm and peak EQE of 18.2% at 646 nm, showing potential in meeting the requirements of display standard.     

High‐Performance Hybrid White Organic Light‐Emitting Diodes with Superior Efficiency/Color Rendering Index/Color Stability and Low Efficiency Roll‐Off Based on a Blue Thermally Activated Delayed Fluorescent Emitter

Thermally activated delayed fluorescence (TADF)‐based white organic light‐emitting diodes (WOLEDs) are highly attractive because the TADF emitters provide a promising alternative route to harvest triplet excitons. One of the major challenges is to achieve superior efficiency/color rendering index/color stability and low efficiency roll‐off simultaneously. In this paper, high‐performance hybrid WOLEDs are demonstrated by employing an efficient blue TADF emitter combined with red and green phosphorescent emitters. The resulting WOLED shows the maximum external quantum efficiency, current efficiency, and power efficiency of 23.0%, 51.0 cd A^?1, and 51.7 lm W^?1, respectively. Moreover, the device exhibits extremely stable electroluminescence spectra with a high color rendering index of 89 and Commission Internationale de L'Eclairage coordinates of (0.438, 0.438) at the practical brightness of 1000 cd m^?2. The achievement of these excellent performances is systematically investigated by versatile experimental and theoretical evidences, from which it is concluded that the utilization of a blue‐green‐red cascade energy transfer structure and the precise manipulation of charges and excitons are the key points. It can be anticipated that this work might be a starting point for further research towards high‐performance hybrid WOLEDs.     

Manipulation of Charge and Exciton Distribution Based on Blue Aggregation‐Induced Emission Fluorophors: A Novel Concept to Achieve High‐Performance Hybrid White Organic Light‐Emitting Diodes

The aggregation‐induced emission (AIE) phenomenon is important in organic light‐emitting diodes (OLEDs), for it can potentially solve the aggregation‐caused quenching problem. However, the performance of AIE fluorophor‐based OLEDs (AIE OLEDs) is unsatisfactory, particularly for deep‐blue devices (CIEy < 0.15). Here, by enhancing the device engineering, a deep‐blue AIE OLED exhibits low voltage (i.e., 2.75 V at 1 cd m^?2), high luminance (17 721 cd m^?2), high efficiency (4.3 lm W^?1), and low efficiency roll‐off (3.6 lm W^?1 at 1000 cd m^?2), which is the best deep‐blue AIE OLED. Then, blue AIE fluorophors, for the first time, have been demonstrated to achieve high‐performance hybrid white OLEDs (WOLEDs). The two‐color WOLEDs exhibit i) stable colors and the highest efficiency among pure‐white hybrid WOLEDs (32.0 lm W^?1); ii) stable colors, high efficiency, and very low efficiency roll‐off; or iii) unprecedented efficiencies at high luminances (i.e., 70.2 cd A^?1, 43.4 lm W^?1 at 10 000 cd m^?2). Moreover, a three‐color WOLED exhibits wide correlated color temperatures (10 690–2328 K), which is the first hybrid WOLED showing sunlight‐style emission. These findings will open a novel concept that blue AIE fluorophors are promising candidates to develop high‐performance hybrid WOLEDs, which have a bright prospect for the future displays and lightings.     

Solvent‐Polarity‐Engineered Controllable Synthesis of Highly Fluorescent Cesium Lead Halide Perovskite Quantum Dots and Their Use in White Light‐Emitting Diodes

Cesium lead halide quantum dots (QDs) have tunable photoluminescence that is capable of covering the entire visible spectrum and have high quantum yields, which make them a new fluorescent materials for various applications. Here, the synthesis of CsPbX₃ (X = Cl, Br, I, or mixed Cl/Br and Br/I) QDs by direct ion reactions in ether solvents is reported, and for the first time the synergetic effects of solvent polarity and reaction temperature on the nucleation and growth of QDs are demonstrated. The use of solvent with a low polarity enables controlled growth of QDs, which facilitates the synthesis of high‐quality CsPbX₃ QDs with broadly tunable luminescence, narrow emission width, and high quantum yield. A QD white LED (WLED) is demonstrated by coating the highly fluorescent green‐emissive CsPbBr₃ QDs together with red phosphors on a blue InGaN chip, which presents excellent warm white light emission with a high rendering index of 93.2 and color temperature of 5447 K, suggesting the potential applications of highly fluorescent cesium lead halide perovskite QDs as an alternative color converter in the fabrication of WLEDs.     

Design Strategy of Blue and Yellow Thermally Activated Delayed Fluorescence Emitters and Their All‐Fluorescence White OLEDs with External Quantum Efficiency beyond 20%

Two thioxanthone‐derived isomeric series of thermally activated delayed fluorescence (TADF) emitters 1,6‐2TPA‐TX/3,6‐2TPA‐TX and 1,6‐2TPA‐TXO/3,6‐2TPA‐TXO are developed for organic light‐emitting diodes (OLEDs). Blue emission devices based on symmetrical 3,6‐2TPA‐TX with common vertical transition route realize an extremely high external quantum efficiency (EQE) of 23.7%, and an ever highest EQE of 24.3% is achieved for yellow emission devices based on 3,6‐2TPA‐TXO by solely changing the sulfur atom valence state of the thioxanthone core. In contrast, their corresponding asymmetric isomers are affected by intramolecular energy transfer and more severely by a nonradiative deactivation pathway, to give much low EQE values (<5%). By utilizing 3,6‐2TPA‐TX as a blue emitter and 3,6‐2TPA‐TXO as a yellow emitter, an ever highest EQE of 20.4% is achieved for all‐fluorescence white OLEDs.