Barrierless Exciton Self-Trapping and Emission Mechanism in Low-Dimensional Copper Halides

Zengshan Xing; Zhicong Zhou; Guohua ZhongChristopher C. S. ChanYanyan LiXinhui ZouJonathan E. HalpertHaibin SuKam Sing Wong

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Barrierless Exciton Self-Trapping and Emission Mechanism in Low-Dimensional Copper Halides

机译：Barrierless Exciton Self-Trapping and Emission Mechanism in Low-Dimensional Copper Halides

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Low-dimensional copper halides having nontoxic elements are attractingincreasing attention for their peculiar emission properties. Self-trappedexcitons (STEs) account for their high photoluminescence quantum yields(PLQYs) with emission that can stretch across the entire visible spectrum.However, intrinsic factors that influence the formation or loss of the emissivespecies in low-dimensional copper halides remain elusive. Here, a comprehensivestudy on the STE formation dynamics of one-dimensional CsCu_2I_3and zero-dimensional Cs_3Cu_2I_5 is presented. It is found from STE kineticanalysis that a slower STE formation demonstrated by the 1D structure is nothindered by a potential barrier, but instead related to the number of phononsreleased in the self-trapping process. It is further revealed that in 1D CsCu_2I_3,the non-radiative recombination of STEs mainly occurs via the intersectionbetween the STE state and the ground state in the configuration coordinatediagram, placing an intrinsic limit on the PLQY at room temperature. Thesefindings show that the STE formation is affected by both the self-trappingdepth and the phonon energy as opposed to a potential barrier in low-dimensionalcopper halides. The better understanding of STE formation and recombinationprocesses provide basis for improving design and performance forbroadband light emitting devices.

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《Advanced functional materials》 |2022年第46期|2207638.1-2207638.9|共9页
作者
Zengshan Xing; Zhicong Zhou; Guohua ZhongChristopher C. S. ChanYanyan LiXinhui ZouJonathan E. HalpertHaibin SuKam Sing Wong;
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作者单位

Department of ChemistryThe Hong Kong University of Science and TechnologyClear Water Bay, Kowloon, Hong Kong, P. R. China;

Department of Physics and William Mong Institute of Nano Scienceand TechnologyThe Hong Kong University of Science and TechnologyClear Water Bay, Kowloon, Hong Kong, P. R. China;

Shenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055, P. R. China;

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barrierless exciton self-trapping; electron–phonon coupling; lowdimensional metal halides; negligible exciton detrapping; non-radiative loss pathway;

Barrierless Exciton Self-Trapping and Emission Mechanism in Low-Dimensional Copper Halides

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