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1.
This work presents a strategy of combining the concepts of localized surface plasmons (LSPs) and core/shell nanostructure configuration in a single perovskite light‐emitting diode (PeLED) to addresses simultaneously the emission efficiency and stability issues facing current PeLEDs' challenges. Wide bandgap n‐ZnO nanowires and p‐NiO are employed as the carrier injectors, and also the bottom/upper protection layers to construct coaxial core/shell heterostructured CsPbBr3 quantum dots LEDs. Through embedding plasmonic Au nanoparticles into the device and thickness optimization of the MgZnO spacer layer, an emission enhancement ratio of 1.55 is achieved. The best‐performing plasmonic PeLED reaches up a luminance of 10 206 cd m?2, an external quantum efficiency of ≈4.626%, and a current efficiency of 8.736 cd A?1. The underlying mechanisms for electroluminescence enhancement are associated with the increased spontaneous emission rate and improved internal quantum efficiency induced by exciton–LSP coupling. More importantly, the proposed PeLEDs, even without encapsulation, present a substantially improved operation stability against water and oxygen degradation (30‐day storage in air ambient, 85% humidity) compared with any previous reports. It is believed that the experimental results obtained will provide an effective strategy to enhance the performance of PeLEDs, which may push forward the application of such kind of LEDs.  相似文献   

2.
Quasi‐2D (Q2D) lead halide perovskites have emerged as promising materials for light‐emitting diodes (LEDs) due to their tunable emission, slowed‐down carrier diffusion, and improved stability. However, they are primarily fabricated through solution methods, which hinders its large‐scale manufacture and practical applications. Physical‐vapor‐deposition (PVD) methods have well demonstrated the capability for reproducible, scalable, and layer‐by‐layer fabrication of high quality organic/inorganic thin films. Herein, for the first time, the full‐evaporation fabrication of organic–inorganic hybrid ((BA)2Csn?1PbnBr3n+1) Q2D–3D PeLEDs is demonstrated. The morphology and crystal phase of the perovskite are controlled from 3D to 2D by modulating material composition, annealing temperature, and film thicknesses. The confinement of carriers in 3D layers and the energy funnel effect are discovered and discussed. Importantly, a record high external quantum efficiency (EQE) of 5.3% based on evaporation method is achieved. Moreover, a centimeter‐scale PeLED (1.5 cm × 2 cm) is obtained. Furthermore, the T50 lifetime of the device with an initial brightness of 100 cd m?2 is found to be 90 min with a thin layer PMMA passivation, which is among the longest for all PVD processed PeLEDs. Overall, this work casts a solid stepping stone towards the fabrication of high‐performance PeLEDs on a large‐scale.  相似文献   

3.
Light‐emitting diodes (LEDs) based on lead halide perovskites demonstrate outstanding optoelectronic properties and are strong competitors for display and lighting applications. While previous halide perovskite LEDs are mainly produced via solution processing, here an all‐vacuum processing method is employed to construct CsPbBr3 LEDs because vacuum processing exhibits high reliability and easy integration with existing OLED facilities for mass production. The high‐throughput combinatorial strategies are further adopted to study perovskite composition, annealing temperature, and functional layer thickness, thus significantly speeding up the optimization process. The best rigid device shows a current efficiency (CE) of 4.8 cd A?1 (EQE of 1.45%) at 2358 cd m?2, and best flexible device shows a CE of 4.16 cd A?1 (EQE of 1.37%) at 2012 cd m?2 with good bending tolerance. Moreover, by choosing NiOx as the hole‐injection layer, the CE is improved to 10.15 cd A?1 and EQE is improved to a record of 3.26% for perovskite LEDs produced by vacuum deposition. The time efficient combinatorial approaches can also be applied to optimize other perovskite LEDs.  相似文献   

4.
All‐inorganic perovskite light‐emitting diodes (LEDs) reveal efficient luminescence with high color purity, but their modest brightness and poor stability are still critical drawbacks. Here, the luminescent efficiency and the stability of perovskite LEDs (PeLEDs) are boosted by antisolvent vapor treatment of CsPbBr3 embedded in a dielectric polymer matrix of polyethylene oxide (PEO). A unique method is developed to obtain high quality CsPbBr3 emitting layers with low defects by controlling their grain sizes. CsPbBr3 in PEO matrix is post‐treated with antisolvent of chloroform (CF), leading to microcrystals with a size of ≈5 µm along the in‐plane direction with active emitting composite of 90%. A device based on CF post‐treatment (CsPbBr3‐PEO‐CF) film displays a brightness of up to 51890 cd m?2 with an external quantum efficiency of 4.76%. CsPbBr3‐PEO‐CF PeLED still maintains 82% of its initial efficiency after 80 h continuous operation in ambient air, which indicates relatively good device stability. This work highlights that film quality is not only key to promoting fluorescence in CsPbBr3, but also to achieving higher performance PeLEDs.  相似文献   

5.
Substantial achievements have been made in green and red perovskite light emitting diodes (PeLEDs) recently. However, blue PeLEDs still lag behind with much lower performances. One of the main reasons is the mass undesirable nonradiative recombination at interfaces and within the perovskite films. In this work, an efficient hole transport bi‐layer structure composed of PSSNa and NiOx is demonstrated to simultaneously inhibit the nonradiative decays between NiOx and perovskite films by reducing NiOx surface defects and improving quasi‐2D perovskite thin film quality by minimizing its pin‐holes and reducing the film roughness. The results show that the dipole feature of PSSNa improves the hole transportation and thus PeLED performances. Moreover, by introducing KBr into the perovskite, its film quality improves and trap states reduce. Eventually, the blue PeLEDs is achieved with a very low turn‐on voltage of 3.31 V accompanied with an external quantum efficiency of 1.45% and a remarkable luminance of 4359 cd m‐2. With further optimization of the perovskite precursor concentration, the highest luminance reaches 5737 cd m‐2, which represents the brightest blue PeLEDs reported to date as far as it is known. Furthermore, the devices also show better spectral stability and operation lifetime as compared to other blue PeLEDs.  相似文献   

6.
This paper reports quantitative correlation of CH3NH3PbBr3 (MAPbBr3) thin film morphology to light emitting diode efficiency parameters. Sequential (spin coating) deposition is used for highly reproducible and dense film morphology of MAPbBr3 thin‐film. In this fabrication process using an orthogonal solvent approach, control of morphology, coverage, thickness, and optical properties in these compact thin‐films is demonstrated. Optical studies show direct correlation between morphology to dynamics of photoluminescence (PL) and absolute PL yield. Perovskite light emitting diodes (PeLEDs) are fabricated from these films to find the best ratio of PbBr2 versus MABr for optimal performance. This study demonstrates PeLEDs with high brightness, ≈1050 cd m?2 at 4.7 V (luminance efficiency ≈0.1 cd A?1), for optimal thin‐film process with state‐of‐the‐art device performance. This quantitative analysis suggests that these state‐of‐the‐art PeLEDs suffer from poor charge carrier balance (≈2%) and out‐coupling efficiency (≈6%). Interestingly, charge carrier balance and PL yield together can explain the change in PeLED efficiency modulation with film morphology. Studies on single carrier devices show that these PeLEDs are electron current dominated and charge carrier balance increases with operating bias voltage.  相似文献   

7.
A specially designed n‐type semiconductor consisting of Ca‐doped ZnO (CZO) nanoparticles is used as the electron transport layer (ETL) in high‐performance multicolor perovskite light‐emitting diodes (PeLEDs) fabricated using an all‐solution process. The band structure of the ZnO is tailored via Ca doping to create a cascade of conduction energy levels from the cathode to the perovskite. This energy band alignment significantly enhances conductivity and carrier mobility in the CZO ETL and enables controlled electron injection, giving rise to sub‐bandgap turn‐on voltages of 1.65 V for red emission, 1.8 V for yellow, and 2.2 V for green. The devices exhibit significantly improved luminance yields and external quantum efficiencies of, respectively, 19 cd A?1 and 5.8% for red emission, 16 cd A?1 and 4.2% for yellow, and 21 cd A?1 and 6.2% for green. The power efficiencies of these multicolor devices demonstrated in this study, 30 lm W?1 for green light‐emitting PeLED, 28 lm W?1 for yellow, and 36 lm W?1 for red are the highest to date reported. In addition, the perovskite layers are fabricated using a two‐step hot‐casting technique that affords highly continuous (>95% coverage) and pinhole‐free thin films. By virtue of the efficiency of the ETL and the uniformity of the perovskite film, high brightnesses of 10 100, 4200, and 16,060 cd m?2 are demonstrated for red, yellow, and green PeLEDs, respectively. The strategy of using a tunable ETL in combination with a solution process pushes perovskite‐based materials a step closer to practical application in multicolor light‐emitting devices.  相似文献   

8.
Introducing extensively excess ammonium halides when forming perovskites has recently been demonstrated as an effective approach to improve the performance of perovskite light‐emitting diodes (PeLEDs). Here, Cs0.17FA0.83PbI2.5Br0.5 is used as a model system to elucidate the impact of introducing excess formamidinium iodide (FAI) on the crystallization process of the perovskite film and operation of the corresponding PeLED. The excess FAI ratio is varied from 0 to 120 mol% and the crystallization process of the perovskite through in situ absorbance, in situ photoluminescence, and ex situ X‐ray diffraction measurements is systematically monitored. The results suggest that excess FAI triggers formation of a compact wide‐bandgap intermediate phase in the as‐deposited film, which then transforms to isolated and highly crystalline perovskite grains upon annealing. Using excitation correlation photoluminescence spectroscopy it is found that excess FAI results in a lower density of deep trap states and therefore a reduction of nonradiative losses in the material. This leads to a greatly enhanced maximum external quantum efficiency (EQE) from 0.25% (stoichiometric) to 12.7% (90 mol% excess). Furthermore, the FAI‐excess perovskite film is optimized with Pb(SCN)2 and 5‐ammonium valeric acid iodide additives and achieve a record radiance of 965 W Sr?1 m?2 for near‐infrared PeLEDs and a high EQE of 17.4%.  相似文献   

9.
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 (Cs1?xRbx)1?yKyPbBr3 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%.  相似文献   

10.
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.  相似文献   

11.
A dual‐phase all‐inorganic composite CsPbBr3‐CsPb2Br5 is developed and applied as the emitting layer in LEDs, which exhibited a maximum luminance of 3853 cd m–2, with current density (CE) of ≈8.98 cd A–1 and external quantum efficiency (EQE) of ≈2.21%, respectively. The parasite of secondary phase CsPb2Br5 nanoparticles on the cubic CsPbBr3 nanocrystals could enhance the current efficiency by reducing diffusion length of excitons on one side, and decrease the trap density in the band gap on the other side. In addition, the introduction of CsPb2Br5 nanoparticles could increase the ionic conductivity by reducing the barrier against the electronic and ionic transport, and improve emission lifetime by decreasing nonradiative energy transfer to the trap states via controlling the trap density. The dual‐phase all‐inorganic CsPbBr3‐CsPb2Br5 composite nanocrystals present a new route of perovskite material for advanced light emission applications.  相似文献   

12.
Organic–inorganic hybrid perovskites (OHPs) are promising emitters for light‐emitting diodes (LEDs) due to the high color purity, low cost, and simple synthesis. However, the electroluminescent efficiency of polycrystalline OHP LEDs (PeLEDs) is often limited by poor surface morphology, small exciton binding energy, and long exciton diffusion length of large‐grain OHP films caused by uncontrolled crystallization. Here, crystallization of methylammonium lead bromide (MAPbBr3) is finely controlled by using a polar solvent‐soluble self‐doped conducting polymer, poly(styrenesulfonate)‐grafted polyaniline (PSS‐g‐PANI), as a hole injection layer (HIL) to induce granular structure, which makes charge carriers spatially confined more effectively than columnar structure induced by the conventional poly(3,4‐ethylenedioythiphene):polystyrenesulfonate (PEDOT:PSS). Moreover, lower acidity of PSS‐g‐PANI than PEDOT:PSS reduces indium tin oxide (ITO) etching, which releases metallic In species that cause exciton quenching. Finally, doubled device efficiency of 14.3 cd A‐1 is achieved for PSS‐g‐PANI‐based polycrystalline MAPbBr3 PeLEDs compared to that for PEDOT:PSS‐based PeLEDs (7.07 cd A‐1). Furthermore, PSS‐g‐PANI demonstrates high efficiency of 37.6 cd A‐1 in formamidinium lead bromide nanoparticle LEDs. The results provide an avenue to both control the crystallization kinetics and reduce the migration of In released from ITO by forming OIP films favorable for more radiative luminescence using the polar solvent‐soluble and low‐acidity polymeric HIL.  相似文献   

13.
Producing efficient blue and deep blue perovskite LEDs (PeLEDs) still represents a significant challenge in optoelectronics. Blue PeLEDs still have problems relating to color, luminance, and structural and electrical stability so new materials are needed to achieve better performance. Recent reports suggest using low n states (n = 1, 2, 3) to achieve blue electroluminescence in Ruddlesden–Popper (RP) perovskite films. However, there are fewer reports on the other quasi-2D structure, Dion–Jacobson (DJ) perovksites, despite their highly desirable optical properties, due to the difficulty in achieving charge injection. To resolve this issue, herein, w e have mixed DJ phase precursors, propane-1,3-diammonium (PDA) bromide into RP phase perovskites and fabricated low-dimensional PeLEDs. It is found that these specific precursors aid in suppressing both the low n (n = 1) and high n (n ≥ 4) quasi-2D RP phases and is an effective strategy in blue-shifting sky-blue RP perovskites into the sub-470 nm region. With optimization of the PDA concentration and device layers, it is achieved an external quantum efficiency of 1.5% at 469 nm and stable electroluminescence for the first deep blue PeLED to be reported using DJ perovskites.  相似文献   

14.
Perovskite lighting-emitting diodes (PeLEDs) with inverted structure have been considered as promising display technology due to their suitable driving schemes with n-type thin-film transistors. However, the defects and imbalanced charge carriers in the CsPbBr3 nanocrystal (NC) PeLED are key hurdles, limiting the performance. Herein, we have successfully doped Zn2+ ions into CsPbBr3 NCs by ligand-assisted reprecipitation method, exhibiting an 85% enhancement of the photoluminescence quantum yield (PLQY). In addition, the optimized energy level alignment via Zn doping facilitates the carrier balance in the devices, improving the efficiencies. The obtained CsPbBr3:Zn-based PeLED reaches a high luminance of 3124 cd/m2 and a maximum external quantum efficiency (EQE) of 0.85%, which are superior to those of CsPbBr3-based PeLED (luminance = 564 cd/m2, EQE = 0.09%). The results demonstrate that Zn doping significantly enhances the performance of PeLED, which increases the potential of these inverted PeLEDs connected with n-type TFTs towards practical applications.  相似文献   

15.
The past few years have seen a significant improvement in the efficiency of organometal halide‐perovskite‐based light‐emitting diodes (PeLEDs). However, poor operation stability of the devices still hinders the commercialization of this technology for practical applications. Despite extensive studies on the degradation mechanisms of perovskite thin films, it remains unclear where and how degradation occurs in a PeLED. Electroabsorption (EA) spectroscopy is applied to study the degradation process of PeLEDs during operation and directly evaluates the stability of each functional layer (i.e., charge transporting layers and light‐emitting layer) by monitoring their unique optical signatures. The EA measurements unambiguously reveal that the degradation of the PeLEDs occurs predominantly in the perovskite layer. With finite‐element method‐based device modeling, it is further revealed that the degradation may initiate from the interface between the perovskite and hole transporting layers and that vacancy, antisite, or interstitial defects can further accelerate this degradation. Inspired by these observations, a surface‐treatment step is introduced to passivate the perovskite surface with phenethylammonium iodide. The passivation leads to a drastic enhancement of the PeLED stability, with the operation lifetime increased from 1.5 to 11.3 h under a current density of 100 mA cm?2.  相似文献   

16.
Making small nanograins in polycrystalline organic–inorganic halide perovskite (OIHP) films is critical to improving the luminescent efficiency in perovskite light‐emitting diodes (PeLEDs). 3D polycrystalline OIHPs have fundamental limitations related to exciton binding energy and exciton diffusion length. At the same time, passivating the defects at the grain boundaries is also critical when the grain size becomes smaller. Molecular additives can be incorporated to shield the nanograins to suppress defects at grain boundaries; however, unevenly distributed molecular additives can cause imbalanced charge distribution and inefficient local defect passivation in polycrystalline OIHP films. Here, a kinetically controlled polycrystalline organic‐shielded nanograin (OSN) film with a uniformly distributed organic semiconducting additive (2,2′,2′′‐(1,3,5‐benzinetriyl)‐tris(1‐phenyl‐1‐H‐benzimidazole), TPBI) is developed mimicking core–shell nanoparticles. The OSN film causes improved photophysical and electroluminescent properties with improved light out‐coupling by possessing a low refractive index. Finally, highly improved electroluminescent efficiencies of 21.81% ph el?1 and 87.35 cd A?1 are achieved with a half‐sphere lens and four‐time increased half‐lifetime in polycrystalline PeLEDs. This strategy to make homogeneous, defect‐healed polycrystalline core–shell‐mimicked nanograin film with better optical out‐coupling will provide a simple and efficient way to make highly efficient perovskite polycrystal films and their optoelectronics devices.  相似文献   

17.
Solution‐processed metal halide perovskites (MHPs) have attracted much attention for applications in light‐emitting diodes (LEDs) due to their wide color gamut, high color purity, tunable emission wavelength, balanced electron/hole transportation, etc. Although MHPs are very tolerant to defects, the defects in solution‐processed perovskite LEDs (PeLEDs) still cause severe nonradiative recombination and device instability. Here, molecular design of additives for dual passivation of both lead and halide defects in perovskites is reported. A bi‐functional additive, 4‐fluorophenylmethylammonium‐trifluoroacetate (FPMATFA), is synthesized by using a simple solution process. The TFA anions and FPMA cations can bond with undercoordinated lead and halide ions, respectively, resulting in dual passivation of both lead and halide defects. In addition, the bulky FPMA group can constrain the grain growth of 3D perovskite, enhancing electron–hole capture rates and radiative recombination rates. As a result, high‐performance PeLEDs with a peak external quantum efficiency reaching 20.9% and emission wavelength at 694 nm are achieved using formamidinium‐cesium lead iodide‐bromide (FA0.33Cs0.67Pb(I0.7Br0.3)3). Furthermore, the operational lifetime of PeLEDs is also greatly improved due to the low trap density in the perovskite film.  相似文献   

18.
The electronic properties, carrier injection, and transport into poly(9,9‐dioctylfluorene) (PFO), PFO end‐capped with hole‐transporting moieties (HTM), PFO–HTM, and PFO end‐capped with electron‐transporting moieties (ETM), PFO–ETM, were investigated. The data demonstrate that charge injection and transport can be tuned by end‐capping with HTM and ETM, without significantly altering the electronic properties of the conjugated backbone. End‐capping with ETM resulted in more closely balanced charge injection and transport. Single‐layer electrophosphorescent light‐emitting diodes (LEDs), fabricated from PFO, PFO–HTM and PFO–ETM as hosts and tris[2,5‐bis‐2′‐(9′,9′‐dihexylfluorene)pyridine‐κ2NC3′]iridium(III ), Ir(HFP)3 as the guest, emitted red light with brightnesses of 2040 cd m–2, 1940 cd m–2 and 2490 cd m–2 at 290 mA cm–2 (16 V) and with luminance efficiencies of 1.4 cd A–1, 1.4 cd A–1 and 1.8 cd A–1 at 4.5 mA cm–2 for PFO, PFO–HTM, and PFO–ETM, respectively.  相似文献   

19.
Perovskite light-emitting diodes (PeLEDs) are advancing because of their superior external quantum efficiencies (EQEs) and color purity. Still, additional work is needed for blue PeLEDs to achieve the same benchmarks as the other visible colors. This study demonstrates an extremely efficient blue PeLED with a 488 nm peak emission, a maximum luminance of 8600 cd m−2, and a maximum EQE of 12.2% by incorporating the double-sided ethane-1,2-diammonium bromide (EDBr2) ligand salt along with the long-chain ligand methylphenylammonium chloride (MeCl). The EDBr2 successfully improves the interaction between 2D perovskite layers by reducing the weak van der Waals interaction and creating a Dion–Jacobson (DJ) structure. Whereas the pristine sample (without EDBr2) is inhibited by small stacking number (n) 2D phases with nonradiative recombination regions that diminish the PeLED performance, adding EDBr2 successfully enables better energy transfer from small n phases to larger n phases. As evidenced by photoluminescence (PL), scanning electron microscopy (SEM), and atomic force microscopy (AFM) characterization, EDBr2 improves the morphology by reduction of pinholes and passivation of defects, subsequently improving the efficiencies and operational lifetimes of quasi-2D blue PeLEDs.  相似文献   

20.
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.  相似文献   

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