Organic-inorganic hybrid perovskites are emerging low-cost emitters with very high color purity, but their low luminescent efficiency is a critical drawback. We boosted the current efficiency (CE) of perovskite light-emitting diodes with a simple bilayer structure to 42.9 candela per ampere, similar to the CE of phosphorescent organic light-emitting diodes, with two modifications: We prevented the formation of metallic lead (Pb) atoms that cause strong exciton quenching through a small increase in methylammonium bromide (MABr) molar proportion, and we spatially confined the exciton in uniform MAPbBr3 nanograins (average diameter = 99.7 nanometers) formed by a nanocrystal pinning process and concomitant reduction of exciton diffusion length to 67 nanometers. These changes caused substantial increases in steady-state photoluminescence intensity and efficiency of MAPbBr3 nanograin layers.
Highly efficient organic/inorganic hybrid perovskite light-emitting diodes (PeLEDs) based on graphene anode are developed for the first time. Chemically inert graphene avoids quenching of excitons by diffused metal atom species from indium tin oxide. The flexible PeLEDs with graphene anode on plastic substrate show good bending stability; they provide an alternative and reliable flexible electrode for highly efficient flexible PeLEDs.
We have achieved high-efficiency polycrystalline perovskite light-emitting diodes (PeLEDs) based on formamidinium (FA) and cesium (Cs) mixed cations without quantum dot synthesis. Uniform single-phase FACs PbBr polycrystalline films were fabricated by one-step formation with various FA:Cs molar proportions; then the influences of chemical composition on film morphology, crystal structure, photoluminescence (PL), and electroluminescence (EL) were systematically investigated. Incorporation of Cs cations in FAPbBr significantly reduced the average grain size (to 199 nm for FA:Cs = 90:10) and trap density; these changes consequently increased PL quantum efficiency (PLQE) and PL lifetime of FACs PbBr films and current efficiency (CE) of PeLEDs. Further increase in Cs molar proportion from 10 mol % decreased crystallinity and purity, increased trap density, and correspondingly decreased PLQE, PL lifetime, and CE. Incorporation of Cs also increased photostability of FACs PbBr films, possibly due to suppressed formation of light-induced metastable states. FACs PbBr PeLEDs show the maximum CE = 14.5 cd A at FA:Cs = 90:10 with very narrow EL spectral width (21-24 nm); this is the highest CE among FA-Cs-based PeLEDs reported to date. This work provides an understanding of the influences of Cs incorporation on the chemical, structural, and luminescent properties of FAPbBr polycrystalline films and a breakthrough to increase the efficiency of FACs PbBr PeLEDs.
Perovskite light-emitting diodes (PeLEDs) based on three-dimensional (3D) polycrystalline perovskites suffer from ion migration, which causes overshoot of luminance over time during operation and reduces its operational lifetime. Here, we demonstrate 3D/2D hybrid PeLEDs with extremely reduced luminance overshoot and 21 times longer operational lifetime than 3D PeLEDs. The luminance overshoot ratio of 3D/2D hybrid PeLED is only 7.4% which is greatly lower than that of 3D PeLED (150.4%). The 3D/2D hybrid perovskite is obtained by adding a small amount of neutral benzylamine to methylammonium lead bromide, which induces a proton transfer from methylammonium to benzylamine and enables crystallization of 2D perovskite without destroying the 3D phase. Benzylammonium in the perovskite lattice suppresses formation of deep-trap states and ion migration, thereby enhances both operating stability and luminous efficiency based on its retardation effect in reorientation.
We introduce a simple, inexpensive, and large-area flexible transparent lamination encapsulation method that uses graphene films with polydimethylsiloxane (PDMS) buffer on polyethylene terephthalate (PET) substrate. The number of stacked graphene layers (nG) was increased from 2 to 6, and 6-layered graphene-encapsulation showed high impermeability to moisture and air. The graphene-encapsulated polymer light emitting diodes (PLEDs) had stable operating characteristics, and the operational lifetime of encapsulated PLEDs increased as nG increased. Calcium oxidation test data confirmed the improved impermeability of graphene-encapsulation with increased nG. As a practical application, we demonstrated large-area flexible organic light emitting diodes (FOLEDs) and transparent FOLEDs that were encapsulated by our polymer/graphene encapsulant.
Metal halide perovskites (MHPs) are being widely studied as a lightabsorber for high-efficiency solar cells. With efforts being made throughout the globe, the power conversion efficiency of MHP solar cells has recently soared up to 25.2%. MHPs are now being spotlighted as a next-generation light-emitter as well. Their high color purity and solution-processability are of particular interest for display applications, which in general benefit from wide color gamut and low-cost high-resolution subpixel patterning. For this reason, research activities on perovskite light-emitting diodes (LEDs) are rapidly growing, and their external quantum efficiencies have been dramatically improved to over 20%. As more and more research groups with different backgrounds are working on these perovskite optoelectronic devices, the demand is growing for standard methods for accurate efficiency measurement that can be agreed upon across the disciplines and, at the same time, can be realized easily in the lab environment with due diligence. Herein, optoelectronic characterization methods are revisited from the viewpoint of MHP solar cells and LEDs. General efficiency measurement practices are first reviewed, common sources of errors are introduced, and guidelines for avoiding or minimizing those errors are then suggested to help researchers in fields develop the best measurement practice.
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.
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-Hbenzimidazole), 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.
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