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Multistep Photoluminescence Decay Reveals Dissociation of Geminate Charge Pairs in Organolead Trihalide Perovskites

机译:多步光致发光衰减揭示了有机油三卤化物钙钛矿中双电荷对的解离。

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Charge carrier dynamics in organolead iodide perovskites is analyzed by employing time-resolved photoluminescence spectroscopy with several ps time resolution. The measurements performed by varying photoexcitation intensity over five orders of magnitude enable separation of photoluminescence components related to geminate and nongeminate charge carrier recombination and to address the dynamics of an isolated geminate electronhole pair. Geminate recombination dominates at low excitation fluence and determines the initial photoluminescence decay. This decay component is remarkably independent of the material structure and experimental conditions. It is demonstrated that dependences of the geminate and nongeminate radiative recombination components on excitation intensity, repetition rate, and temperature, are hardly compatible with carrier trapping and exciton dissociation models. On the basis of semiclassical and quantum mechanical numerical calculation results, it is argued that the fast photoluminescence decay originates from gradual spatial separation of photogenerated weakly bound geminate charge pairs.
机译:通过使用具有几ps时间分辨率的时间分辨光致发光光谱法分析了有机碘化钙钛矿中的载流子动力学。通过在五个数量级上改变光激发强度来进行测量,可以分离出与发芽和非发芽电荷载流子重组有关的光致发光组分,并解决了孤立的发芽电子空穴对的动力学问题。萌芽重组在低激发通量下占主导地位,并确定初始光致发光衰减。该衰减分量明显与材料结构和实验条件无关。结果表明,成对的和非成对的辐射复合成分对激发强度,重复频率和温度的依赖性几乎与载流子俘获和激子离解模型不兼容。根据半经典和量子力学数值计算结果,认为快速的光致发光衰减源于光生弱结合的成对电荷对的逐渐空间分离。

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