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  • Low‐Temperature Absorption,...
    Diroll, Benjamin T.; Zhou, Hua; Schaller, Richard D.

    Advanced functional materials, July 25, 2018, Letnik: 28, Številka: 30
    Journal Article

    The absorption and photoluminescence, both steady‐state and time‐resolved, of CsPbX3 (X = Cl, Br, I) nanocrystals are reported at temperatures ranging from 3 to 300 K. These measurements offer a unique window into the fundamental properties of this class of materials which is considered promising for light‐emitting and detection devices. The bandgaps are shown to increase from low to high temperature, and none of the examined cesium‐based perovskite nanocrystals exhibit a bandgap discontinuity in this temperature range suggesting constant crystal phase. Time‐resolved measurements show that the radiative lifetime of the band‐edge emission depends strongly on the halide ion and increases with heating. The increasing lifetime at higher temperatures is attributed primarily to free carriers produced from exciton fission, corroborated by the prevalence of excitonic character in absorption. The results particularly highlight many of the similarities in physical properties, such as low exciton binding energy and long lifetime, between CsPbI3 and hybrid organic–inorganic plumbotrihalide perovskites. Temperature‐dependent optical studies of CsPbX3 (X = Cl, Br, I) nanocrystals in the bulk‐like size regime demonstrate the bright nature of the lowest emitting state of this class of materials. Low‐temperature absorption measurements directly reveal the composition‐dependent exciton binding energy. Dynamic measurements strongly suggest increased lifetimes at higher temperatures are due to exciton fission.