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      Triammonium Molecular Tripods as Organic Building Blocks for Hybrid Perovskite Solar Cells

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          Abstract

          Considerable efforts have been devoted to the development of new organic‐inorganic hybrid perovskites as well as their passivation‐layer materials to improve the performance of solution‐processable thin‐film solar cells for practical applications. For this purpose, monocations, such as monoammonium ions, have been studied extensively as organic building blocks. Herein, a new class of cationic molecules featuring a triptycene framework is introduced, to which three ammonium ions are attached close to each other. Inspired by the previous finding that 1,8,13‐trisubstituted triptycenes have an excellent ability to form 2D assemblies, two derivatives with ammonium ion groups at these positions are synthesized, linked either directly or via methylene spacers. Hybrid perovskites with different dimensionalities in terms of the inorganic octahedral units were prepared by reaction of the triammonium‐appended triptycene tripods with PbI 2, however, the optoelectronic properties obtained were unsatisfactory. Even so, the triammonium‐containing triptycene tripod having methylene spacers was shown to serve as a good passivation layer for perovskites solar cells (PSCs), leading to improvements in power conversion efficiency and long‐term stability. Given the large degree of design freedom, triptycene tripods merit further investigation as a new motif in the development of surface‐passivation materials for PSCs.

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          Most cited references42

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          Surface passivation of perovskite film for efficient solar cells

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            Solar cells. Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals.

            The fundamental properties and ultimate performance limits of organolead trihalide MAPbX3 (MA = CH3NH3(+); X = Br(-) or I(-)) perovskites remain obscured by extensive disorder in polycrystalline MAPbX3 films. We report an antisolvent vapor-assisted crystallization approach that enables us to create sizable crack-free MAPbX3 single crystals with volumes exceeding 100 cubic millimeters. These large single crystals enabled a detailed characterization of their optical and charge transport characteristics. We observed exceptionally low trap-state densities on the order of 10(9) to 10(10) per cubic centimeter in MAPbX3 single crystals (comparable to the best photovoltaic-quality silicon) and charge carrier diffusion lengths exceeding 10 micrometers. These results were validated with density functional theory calculations.
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              Pseudo-halide anion engineering for α-FAPbI3 perovskite solar cells

              Metal halide perovskites of the general formula ABX3-where A is a monovalent cation such as caesium, methylammonium or formamidinium; B is divalent lead, tin or germanium; and X is a halide anion-have shown great potential as light harvesters for thin-film photovoltaics1-5. Among a large number of compositions investigated, the cubic α-phase of formamidinium lead triiodide (FAPbI3) has emerged as the most promising semiconductor for highly efficient and stable perovskite solar cells6-9, and maximizing the performance of this material in such devices is of vital importance for the perovskite research community. Here we introduce an anion engineering concept that uses the pseudo-halide anion formate (HCOO-) to suppress anion-vacancy defects that are present at grain boundaries and at the surface of the perovskite films and to augment the crystallinity of the films. The resulting solar cell devices attain a power conversion efficiency of 25.6 per cent (certified 25.2 per cent), have long-term operational stability (450 hours) and show intense electroluminescence with external quantum efficiencies of more than 10 per cent. Our findings provide a direct route to eliminate the most abundant and deleterious lattice defects present in metal halide perovskites, providing a facile access to solution-processable films with improved optoelectronic performance.
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                Author and article information

                Contributors
                (View ORCID Profile)
                Journal
                Small Structures
                Small Structures
                Wiley
                2688-4062
                2688-4062
                March 2024
                February 2024
                March 2024
                : 5
                : 3
                Affiliations
                [1 ] Laboratory for Chemistry and Life Science Institute of Innovative Research Tokyo Institute of Technology 4259 Nagatsuta Midori‐ku Yokohama 226‐8501 Japan
                [2 ] Department of Chemical Science and Engineering School of Materials and Chemical Technology Tokyo Institute of Technology 4259 Nagatsuta Midori‐ku Yokohama 226‐8501 Japan
                [3 ] Department of Applied Chemistry Graduate School of Engineering Osaka University 2‐1 Yamadaoka Suita Osaka 565‐0871 Japan
                [4 ] Innovative Catalysis Science Division Institute for Open and Transdisciplinary Research Initiatives (ICS‐OTRI) Osaka University 1‐1 Yamadaoka Suita Osaka 565‐0871 Japan
                [5 ] Precursory Research for Embryonic Science and Technology (PRESTO) Japan Science and Technology Agency 4‐1‐8 Honcho Kawaguchi Saitama 332‐0012 Japan
                [6 ] Application laboratory Rigaku Corporation 3‐9‐12, Matsubara‐cho Akishima‐shi Tokyo 196‐8666 Japan
                [7 ] Living Systems Materialogy (LiSM) Research Group International Research Frontiers Initiative (IRFI) Tokyo Institute of Technology 4259 Nagatsuta Midori‐ku Yokohama 226‐8501 Japan
                Article
                10.1002/sstr.202300411
                0ae05ade-fce8-4669-a117-ead2c0c51249
                © 2024

                http://creativecommons.org/licenses/by/4.0/

                http://creativecommons.org/licenses/by/4.0/

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