biostudies-literatureZhang MNational Natural Science Foundation of ChinaNational Natural Science Foundation of China (National Science Foundation of China)Taishan Scholar Foundation of Shandong Province4890https://www.ebi.ac.uk/biostudies/studies/S-EPMC8361204biostudies-literatureUnknown12(1)Low-dimensional hybrid perovskites have demonstrated excellent performance as white-light emitters. The broadband white emission originates from self-trapped excitons (STEs). Since the mechanism of STEs formation in perovskites is still not clear, preparing new low-dimensional white perovskites relies mostly on screening lots of intercalated organic molecules rather than rational design. Here, we report an atom-substituting strategy to trigger STEs formation in layered perovskites. Halogen-substituted phenyl molecules are applied to synthesize perovskite crystals. The halogen-substituents will withdraw electrons from the branched chain (-R-NH₃⁺) of the phenyl molecule. This will result in positive charge accumulation on -R-NH₃⁺, and thus stronger Coulomb force of bond (-R-NH₃⁺)-(PbBr₄^2-), which facilitates excitons self-trapping. Our designed white perovskites exhibit photoluminescence quantum yield of 32%, color-rendering index of near 90 and chromaticity coordinates close to standard white-light. Our joint experiment-theory study provides insights into the STEs formation in perovskites and will benefit tailoring white perovskites with boosting performance.Nature communicationsMolecular engineering towards efficientwhite-light-emitting perovskite.PMC83612049206111321905154Li HKaghazchi PZhang MZhang LZhang SZhang QYaqoob NYin ZWang LXing JZhao LXie JWang XZhang CXu WfalseMolecular engineering towards efficientwhite-light-emitting perovskite.Low-dimensional hybrid perovskites have demonstrated excellent performance as white-light emitters. The broadband white emission originates from self-trapped excitons (STEs). Since the mechanism of STEs formation in perovskites is still not clear, preparing new low-dimensional white perovskites relies mostly on screening lots of intercalated organic molecules rather than rational design. Here, we report an atom-substituting strategy to trigger STEs formation in layered perovskites. Halogen-substituted phenyl molecules are applied to synthesize perovskite crystals. The halogen-substituents will withdraw electrons from the branched chain (-R-NH₃⁺) of the phenyl molecule. This will result in positive charge accumulation on -R-NH₃⁺, and thus stronger Coulomb force of bond (-R-NH₃⁺)-(PbBr₄^2-), which facilitates excitons self-trapping. Our designed white perovskites exhibit photoluminescence quantum yield of 32%, color-rendering index of near 90 and chromaticity coordinates close to standard white-light. Our joint experiment-theory study provides insights into the STEs formation in perovskites and will benefit tailoring white perovskites with boosting performance.2021-01-01T00:00:00Z2021 Aug2024-11-14T01:23:32.848Z2022-02-11T08:37:16.476ZS-EPMC83612043438545110.1038/s41467-021-25132-2