Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways
Global Analysis of Perovskite Photophysics Reveals Importance of Geminate Pathways
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DOI：
10.1021/acs.jpcc.6b11547
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发表时间：
2017-01
影响因子：
3.7
通讯作者：
Lydia H Manger;M. Rowley;Yongping Fu;Alexander K. Foote;Morgan T. Rea;S. Wood;Song Jin;J. C. Wright;R. Goldsmith
中科院分区：
文献类型：
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作者：
Lydia H Manger;M. Rowley;Yongping Fu;Alexander K. Foote;Morgan T. Rea;S. Wood;Song Jin;J. C. Wright;R. Goldsmith
有机-无机杂化钙钛矿显示出理想的物理行为和从高效光致发光到激光的有前途的应用，但激发态物种的基本性质仍在争论中。我们收集了时间分辨的光致发光的单晶纳米片的甲基铵碘化铅钙钛矿（MAPbI 3）的激发在一定范围内的能量密度和重复率，以提供一个更完整的电子物理图片。一个根本不同的方式来模拟量子物理学的发展，依赖于非归一化的衰变，全球分析了大量的条件，并列入稳态行为，这些细节是至关重要的捕捉观察到的行为。这些额外的限制需要包括空间相关的对沿着与自由载流子和陷阱，证明了我们的综合分析的重要性。对孪晶和非孪晶途径的模拟表明，孪晶过程在高载流子密度和较早的时间内占主导地位。
Hybrid organic–inorganic perovskites demonstrate desirable photophysical behaviors and promising applications from efficient photovoltaics to lasing, but the fundamental nature of excited state species is still under debate. We collected time-resolved photoluminescence of single-crystal nanoplates of methylammonium lead iodide perovskite (MAPbI3) with excitation over a range of fluences and repetition rates to provide a more complete photophysical picture. A fundamentally different way of simulating the photophysics is developed that relies on unnormalized decays, global analysis over a large array of conditions, and inclusion of steady-state behavior; these details are critical to capturing observed behaviors. These additional constraints require inclusion of spatially correlated pairs along with free carriers and traps, demonstrating the importance of our comprehensive analysis. Modeling geminate and nongeminate pathways shows that geminate processes are dominant at high carrier densities and early time...