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      Reducing Nonradiative Losses in Perovskite LEDs through Atomic Layer Deposition of Al 2O 3 on the Hole-Injection Contact

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          Abstract

          Halide perovskite light-emitting diodes (PeLEDs) exhibit great potential for use in next-generation display technologies. However, scale-up will be challenging due to the requirement of very thin transport layers for high efficiencies, which often present spatial inhomogeneities from improper wetting and drying during solution processing. Here, we show how a thin Al 2O 3 layer grown by atomic layer deposition can be used to preferentially cover regions of imperfect hole transport layer deposition and form an intermixed composite with the organic transport layer, allowing hole conduction and injection to persist through the organic hole transporter. This has the dual effect of reducing nonradiative recombination at the heterojunction and improving carrier selectivity, which we infer to be due to the inhibition of direct contact between the indium tin oxide and perovskite layers. We observe an immediate improvement in electroluminescent external quantum efficiency in our p-i-n LEDs from an average of 9.8% to 13.5%, with a champion efficiency of 15.0%. The technique uses industrially available equipment and can readily be scaled up to larger areas and incorporated in other applications such as thin-film photovoltaic cells.

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          Efficient hybrid solar cells based on meso-superstructured organometal halide perovskites.

          The energy costs associated with separating tightly bound excitons (photoinduced electron-hole pairs) and extracting free charges from highly disordered low-mobility networks represent fundamental losses for many low-cost photovoltaic technologies. We report a low-cost, solution-processable solar cell, based on a highly crystalline perovskite absorber with intense visible to near-infrared absorptivity, that has a power conversion efficiency of 10.9% in a single-junction device under simulated full sunlight. This "meso-superstructured solar cell" exhibits exceptionally few fundamental energy losses; it can generate open-circuit photovoltages of more than 1.1 volts, despite the relatively narrow absorber band gap of 1.55 electron volts. The functionality arises from the use of mesoporous alumina as an inert scaffold that structures the absorber and forces electrons to reside in and be transported through the perovskite.
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            Atomic layer deposition: an overview.

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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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                Author and article information

                Journal
                ACS Nano
                ACS Nano
                nn
                ancac3
                ACS Nano
                American Chemical Society
                1936-0851
                1936-086X
                15 February 2023
                28 February 2023
                : 17
                : 4
                : 3289-3300
                Affiliations
                []Clarendon Laboratory, Department of Physics, University of Oxford , Parks Road, Oxford, OX1 3PU, U.K.
                Author notes
                Author information
                https://orcid.org/0000-0001-7098-615X
                https://orcid.org/0000-0003-3518-173X
                https://orcid.org/0000-0003-1512-2046
                https://orcid.org/0000-0003-4572-3459
                https://orcid.org/0000-0002-1726-7110
                https://orcid.org/0000-0002-3897-7963
                https://orcid.org/0000-0003-2578-9645
                https://orcid.org/0000-0001-8511-790X
                Article
                10.1021/acsnano.2c04786
                9979650
                36790329
                747039aa-2aa2-4f1d-b472-d61333daec0e
                © 2023 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 16 May 2022
                : 10 February 2023
                Funding
                Funded by: H2020 Leadership in Enabling and Industrial Technologies, doi 10.13039/100010668;
                Award ID: 861985
                Funded by: University of Oxford, doi 10.13039/501100000769;
                Award ID: NA
                Funded by: Engineering and Physical Sciences Research Council, doi 10.13039/501100000266;
                Award ID: EP/S004947/1
                Categories
                Article
                Custom metadata
                nn2c04786
                nn2c04786

                Nanotechnology
                perovskite,light-emitting diode,atomic layer deposition,area selective,efficiency
                Nanotechnology
                perovskite, light-emitting diode, atomic layer deposition, area selective, efficiency

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