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1.
The reported NiOx interfacial layers in blue perovskite light-emitting diodes (PeLEDs) usually require high-temperature annealing and complex interface modification. Herein, we report a kind of uniform NiOx anode interfacial layer induced by H2O treatment, which effectively enhances the brightness and light-emitting efficiency of blue PeLEDs simultaneously. Compared to the as-prepared NiOx anode interfacial layer, H2O treatment renders uniform and pinhole-free NiOx morphology. The solution-processed perovskite blue emissive layer prepared atop the H2O-treated NiOx interfacial layer demonstrates enhanced photoluminescent property and superior morphology with low trap density. The blue PeLEDs employing H2O-treated NiOx as anode interfacial layer show a maximum luminance of 9052 cd/m2 and a maximum external quantum efficiency (EQE) of 1.80%, whereas the control device based on the as-prepared NiOx anode interfacial layer merely exhibits a maximum luminance of 3850 cd/m2 and an EQE of 0.88%, leading to about 135% and 104% increase in brightness and efficiency, respectively. The PeLEDs emit pure blue light with emission peak located at 482 nm and demonstrate superior spectral stability under different driving voltages and operating time.  相似文献   

2.
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   

3.
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   

4.
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   

5.
Ruddlesden–Popper phase (RP‐phase) perovskites that consist of 2D perovskite slabs interleaved with bulky organic ammonium (OA) are favorable for light‐emitting diodes (LEDs). The critical limitation of LED applications is that the insulating OA arranged in a preferred orientation limits charge transport. Therefore, the ideal solution is to achieve a randomly connected structure that can improve charge transport without hampering the confinement of the electron–hole pair. Here, a structurally modulated RP‐phase metal halide perovskite (MHP), (PEA)2(CH3NH3)m?1PbmBr3m+1 is introduced to make the randomly oriented RP‐phase unit and ensure good connection between them by applying modified nanocrystal pinning, which leads to an increase in the efficiency of perovskite LEDs (PeLEDs). The randomly connected RP‐phase MHP forces contact between inorganic layers and thereby yields efficient charge transport and radiative recombination. Combined with an optimal dimensionality, (PEA)2(CH3NH3)2Pb3Br10, the structurally modulated RP‐phase MHP exhibits increased photoluminescence quantum efficiency, from 0.35% to 30.3%, and their PeLEDs show a 2,018 times higher current efficiency (20.18 cd A?1) than in the 2D PeLED (0.01 cd A?1) and 673 times than in the 3D PeLED (0.03 cd A?1) using the same film formation process. This approach provides insight on how to solve the limitation of RP‐phase MHP for efficient PeLEDs.  相似文献   

6.
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.  相似文献   

7.
Solution‐processed oxide thin films are actively pursued as hole‐injection layers (HILs) in quantum‐dot light‐emitting diodes (QLEDs), aiming to improve operational stability. However, device performance is largely limited by inefficient hole injection at the interfaces of the oxide HILs and high‐ionization‐potential organic hole‐transporting layers. Solution‐processed NiOx films with a high and stable work function of ≈5.7 eV achieved by a simple and facile surface‐modification strategy are presented. QLEDs based on the surface‐modified NiOx HILs show driving voltages of 2.1 and 3.3 V to reach 1000 and 10 000 cd m?2, respectively, both of which are the lowest among all solution‐processed LEDs and vacuum‐deposited OLEDs. The device exhibits a T95 operational lifetime of ≈2500 h at an initial brightness of 1000 cd m?2, meeting the commercialization requirements for display applications. The results highlight the potential of solution‐processed oxide HILs for achieving efficient‐driven and long‐lifetime QLEDs.  相似文献   

8.
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   

9.
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   

10.
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   

11.
Organic–inorganic hybrid perovskites have realized a high power conversion efficiency (PCE) in both n–i–p and p–i–n device configurations. However, since the p–i–n structure exempts the sophisticated processing of charge‐transporting layers, it seems to possess better potential for practical applications than the n–i–p one. Currently, the inorganic NiOx is the most prevailing hole‐transporting layer (HTL) used in p–i–n perovskite solar cells. Nevertheless, defects might exist on its surface to influence the charge transfer/extraction across the interface with perovskite and to affect the quality of the perovskite film grown on it. Herein, two novel [7]helicenes with stable open‐shell singlet biradical ground states at room temperature are demonstrated as an effective surface modifier of the NiOx HTL. Their nonpolar feature effectively promotes the crystallinity of the perovskite film grown on them; meanwhile, their unique partial biradical character seems to provide a certain degree of defect passivation function at the perovskite interface to facilitate interfacial charge transfer/extraction. As a result, both 1ab‐ and 1bb‐modifed devices yield a PCE of >18%, exceeding the value (15.6%) of the control device using a sole NiOx HTL, and the maximum PCE can reach 19%. Detailed characterizations are carefully conducted to understand the underlying reasons behind such enhancement.  相似文献   

12.
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.  相似文献   

13.
The buried interface has important effect on carrier extraction and nonradiative recombination of perovksite solar cells (PSCs). Herein, to inactivate the buried interfacial defects of perovskite and boost the crystallization quality of perovskite film, 3-amino-1-adamantanol (AAD) serves as a pre-buried interface modifier on nickel oxide (NiOx) surface to regulate the nucleation and crystallization process of perovskite precursor. The amino and hydroxyl groups in AAD molecule can synchronously coordinate with nickel ion (Ni3+) in NiOx and lead ion in perovskite, respectively. The dual action favors the ordered arrangement of AAD molecules between NiOx and perovskite, which not only enhances hole extraction in hole transport layer, but also provides active sites for homogeneous nucleation. Furthermore, AAD modifier blocks the unfavorable reaction between Ni3+ and perovskite, and effectively passivates the buried interfacial defects. The optimal inverted PSCs achieve a champion power conversion efficiency of 22.21% with negligible hysteresis, favorable thermal, optical, and long-term stability. Thus, this strategy of modulating perovskite nucleation and crystallization by pre-buried modifier is feasible for achieving efficient and stable inverted perovskite solar cells.  相似文献   

14.
Four monodisperse starburst oligomers bearing a 4,4′,4″‐tris(carbazol‐9‐yl)‐triphenylamine (TCTA) core and six oligofluorene arms are synthesized and characterized. The lengths of oligofluorene arms vary from one to four fluorene units, giving the starburst oligomers molecular weights ranging from 3072 to 10 068 Da (1 Da = 1.66 × 10–27 kg). All of the starburst oligomers have good film‐forming capabilities, and display bright, deep‐blue fluorescence (λmax = 395–416 nm) both in solution and in the solid state, with the quantum efficiencies of the films (ΦPL) varying between 27 and 88 %. Electrochemical studies demonstrate that these materials have large energy gaps, and are stable for both p‐doping and n‐doping processes. Electroluminescent devices are successfully fabricated using these materials as hole‐transporting emitters, and emit deep‐blue light. Devices with luminance values up to 1025 cd m–2 at 11 V and luminous efficiencies of 0.47 cd A–1 at 100 cd m–2 have been produced, which translates to an external quantum efficiency of 1.4 %. In addition, these large‐energy‐gap starburst oligomers are good host materials for red electrophosphorescence. The luminance of the red electrophosphorescent devices is as high as 4452 cd m–2, with a luminous efficiency of 4.31 cd A–1 at 15 mA cm–2: This value is much higher than those obtained from the commonly used hole‐transporting materials, such as poly(vinyl carbazole) (PVK) (1.10 cd A–1 at 16 mA cm–2).  相似文献   

15.
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   

16.
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   

17.
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   

18.
Perovskite light emitting diodes (PeLEDs) have reached external quantum efficiencies (EQEs) over 21%. Their EQE, however, drops at increasing current densities (J) and their lifetime is still limited to just a few hours. The mechanisms leading to EQE roll‐off and device instability require thorough investigation. Here, improvement in EQE, EQE roll‐off, and lifetime of PeLEDs is demonstrated by tuning the balance of electron/hole transport into a mixed 2D/3D perovskite emissive layer. The mixed 2D/3D perovskite layer induces exciton confinement and beneficially influences the electron/hole distribution inside the perovskite layer. By tuning the electron injection to match the hole injection in such active layer, a nearly flat EQE for J = 0.1–200 mA cm?2, a reduced EQE roll‐off until J = 250 mA cm?2, and a half‐lifetime of ≈47 h at J = 10 mA cm?2 is reached. A model is also proposed to explain these improvements that account for the spatial electron/hole distributions.  相似文献   

19.
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   

20.
Novel fluorene‐based compounds, TCPC‐6 and TCPC‐4, with rigid central spirobifluorene cores and peripheral carbazole groups are synthesized using the Suzuki coupling reaction. The optical, electrochemical, and thermal properties of these compounds are characterized. The compounds show strong deep‐blue emission both in solution and as thin films. Both TCPC‐6 and TCPC‐4 exhibit amorphous morphologies in the solid state with high glass transition temperatures (Tg) of 108 and 143 °C, respectively. Atomic force microscopy (AFM) measurements indicate that high‐quality amorphous films of these novel compounds can be prepared by spin‐coating. The oxidation potentials of TCPC‐6 and TCPC‐4 are significant lower than that of model compounds without peripheral carbazole groups, which suggests that these compounds have relatively high highest occupied molecular orbital (HOMO) energy levels and better hole‐injection capabilities. Light‐emitting devices fabricated by spin‐coating films of these molecules exhibit deep‐blue emission with Commission Internationale de l'Eclairage (CIE) chromaticity coordinates (x, y) of (0.16, 0.05); the devices fabricated using spin‐coated TCPC‐6 and TCPC‐4 layers exhibit high luminance efficiencies of 1.35 and 0.90 cd A–1 (with external quantum efficiencies of 3.72 and 2.47 %), respectively.  相似文献   

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