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      Large-area and efficient perovskite light-emitting diodes via low-temperature blade-coating

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          Abstract

          Large-area light-emitting diodes (LEDs) fabricated by mass-production techniques are needed for low-cost flat-panel lighting. Nevertheless, it is still challenging to fabricate efficient large-area LEDs using organic small molecules (OLEDs), quantum dots (QLEDs), polymers (PLEDs), and recently-developed hybrid perovskites (PeLEDs) due to difficulties controlling film uniformity. To that end, we report sol-gel engineering of low-temperature blade-coated methylammonium lead iodide (MAPbI 3) perovskite films. The precipitation, gelation, aging, and phase transformation stages are dramatically shortened by using a diluted, organoammonium-excessed precursor, resulting in ultra-flat large-area films (54 cm 2) with roughness reaching 1 nm. The external quantum efficiency of doctor-bladed PeLEDs reaches 16.1%, higher than that of best-performing blade-coated OLEDs, QLEDs, and PLEDs. Furthermore, benefitting from the throughput of the blade-coating process and cheap materials, the expected cost of the emissive layer is projected to be as low as 0.02 cents per cm 2, emphasizing its application potential.

          Abstract

          Fabrication of efficient large-area perovskite light emitting diodes catering towards mass-production is hampered by the difficulty in getting homogenous uniform films and the high cost. Here, the authors demonstrate sol-gel engineering of low-temperature blade-coated perovskite films which can overcome these limitations.

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          Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent

          Metal halide perovskite materials are an emerging class of solution-processable semiconductors with considerable potential for use in optoelectronic devices1-3. For example, light-emitting diodes (LEDs) based on these materials could see application in flat-panel displays and solid-state lighting, owing to their potential to be made at low cost via facile solution processing, and could provide tunable colours and narrow emission line widths at high photoluminescence quantum yields4-8. However, the highest reported external quantum efficiencies of green- and red-light-emitting perovskite LEDs are around 14 per cent7,9 and 12 per cent8, respectively-still well behind the performance of organic LEDs10-12 and inorganic quantum dot LEDs13. Here we describe visible-light-emitting perovskite LEDs that surpass the quantum efficiency milestone of 20 per cent. This achievement stems from a new strategy for managing the compositional distribution in the device-an approach that simultaneously provides high luminescence and balanced charge injection. Specifically, we mixed a presynthesized CsPbBr3 perovskite with a MABr additive (where MA is CH3NH3), the differing solubilities of which yield sequential crystallization into a CsPbBr3/MABr quasi-core/shell structure. The MABr shell passivates the nonradiative defects that would otherwise be present in CsPbBr3 crystals, boosting the photoluminescence quantum efficiency, while the MABr capping layer enables balanced charge injection. The resulting 20.3 per cent external quantum efficiency represents a substantial step towards the practical application of perovskite LEDs in lighting and display.
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            Bright light-emitting diodes based on organometal halide perovskite.

            Solid-state light-emitting devices based on direct-bandgap semiconductors have, over the past two decades, been utilized as energy-efficient sources of lighting. However, fabrication of these devices typically relies on expensive high-temperature and high-vacuum processes, rendering them uneconomical for use in large-area displays. Here, we report high-brightness light-emitting diodes based on solution-processed organometal halide perovskites. We demonstrate electroluminescence in the near-infrared, green and red by tuning the halide compositions in the perovskite. In our infrared device, a thin 15 nm layer of CH3NH3PbI(3-x)Cl(x) perovskite emitter is sandwiched between larger-bandgap titanium dioxide (TiO2) and poly(9,9'-dioctylfluorene) (F8) layers, effectively confining electrons and holes in the perovskite layer for radiative recombination. We report an infrared radiance of 13.2 W sr(-1) m(-2) at a current density of 363 mA cm(-2), with highest external and internal quantum efficiencies of 0.76% and 3.4%, respectively. In our green light-emitting device with an ITO/PEDOT:PSS/CH3NH3PbBr3/F8/Ca/Ag structure, we achieved a luminance of 364 cd m(-2) at a current density of 123 mA cm(-2), giving external and internal quantum efficiencies of 0.1% and 0.4%, respectively. We show, using photoluminescence studies, that radiative bimolecular recombination is dominant at higher excitation densities. Hence, the quantum efficiencies of the perovskite light-emitting diodes increase at higher current densities. This demonstration of effective perovskite electroluminescence offers scope for developing this unique class of materials into efficient and colour-tunable light emitters for low-cost display, lighting and optical communication applications.
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              Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes.

              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.
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                Author and article information

                Contributors
                zhengguo@ustc.edu.cn
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                8 January 2021
                8 January 2021
                2021
                : 12
                : 147
                Affiliations
                [1 ]GRID grid.59053.3a, ISNI 0000000121679639, Hefei National Laboratory for Physical Science at the Microscale, Department of Physics, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, , University of Science and Technology of China, ; Hefei, Anhui 230026 China
                [2 ]GRID grid.10698.36, ISNI 0000000122483208, Department of Applied Physical Sciences, , University of North Carolina at Chapel Hill, ; Chapel Hill, NC 27599 USA
                Author information
                http://orcid.org/0000-0002-7087-4999
                http://orcid.org/0000-0002-9810-2448
                http://orcid.org/0000-0002-0509-8778
                http://orcid.org/0000-0001-6646-1166
                Article
                20433
                10.1038/s41467-020-20433-4
                7794572
                33420040
                c67c9976-5d85-486a-b18b-d1349fcb640d
                © The Author(s) 2021

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 5 August 2020
                : 11 November 2020
                Funding
                Funded by: FundRef https://doi.org/10.13039/501100001809, National Natural Science Foundation of China (National Science Foundation of China);
                Award ID: 51872274
                Award Recipient :
                Funded by: Fundamental Research Funds for the Central Universities (WK2060190053)
                Categories
                Article
                Custom metadata
                © The Author(s) 2021

                Uncategorized
                electronic devices,lasers, leds and light sources
                Uncategorized
                electronic devices, lasers, leds and light sources

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