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• W4229044006 abstract "Given their comparatively narrow band gap, mixed Pb-Sn iodide perovskites are interesting candidates for bottom cells in all-perovskite tandems or single junction solar cells, and their luminescence around 900 nm offers great potential for near-infrared optoelectronics. Here, we investigate mixed FAPb1-xSnxI3 offering the first accurate determination of the crystal structure over a temperature range from 293 to 100 K. We demonstrate that all compositions exhibit a cubic structure at room temperature and undergo at least two transitions to lower symmetry tetragonal phases upon cooling. Using density functional theory (DFT) calculations based on these structures, we subsequently reveal that the main impact on the band gap bowing is the different energy of the s and p orbital levels derived from Pb and Sn. In addition, this energy mismatch results in strongly composition-dependent luminescence characteristics. Whereas neat and Sn-rich compounds exhibit bright and narrow emission with a clean band gap, Sn-poor compounds intrinsically suffer from increased carrier recombination mediated by in-gap states, as evidenced by the appearance of pronounced low-energy photoluminescence upon cooling. This study is the first to link experimentally determined structures of FAPb1-xSnxI3 with the electronic properties, and we demonstrate that optoelectronic applications based on Pb-Sn iodide compounds should employ Sn-rich compositions." @default.
• W4229044006 created "2022-05-08" @default.
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• W4229044006 date "2022-05-05" @default.
• W4229044006 modified "2023-10-16" @default.
• W4229044006 title "Compositional Variation in FAPb_1–<i>x</i>Sn_<i>x</i>I₃ and Its Impact on the Electronic Structure: A Combined Density Functional Theory and Experimental Study" @default.
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• W4229044006 doi "https://doi.org/10.1021/acsami.2c00889" @default.
• W4229044006 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/35512221" @default.
• W4229044006 hasPublicationYear "2022" @default.
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