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揭示浅陷阱、深陷阱与俄歇陷阱在三阳离子钙钛矿中电荷载流子复合的作用

Unraveling the Roles of Shallow, Deep and Auger Trapping in Charge Carrier Recombination in Triple-Cation Perovskites

Jitendra Kumar, Thomas Kirchartz, Alexandr Marunchenko, Alexander Kiligaridis, Shraddha M. Rao, Shivam Singh, Ankur Yadav, Monojit Bag, Yana Vaynzof, Ivan G. Scheblykin

arXiv 2608.14368首次发表:更新:

AI 中文总结

本研究结合时间分辨光致发光等测量构建统一模型,揭示三阳离子钙钛矿中浅/深陷阱与俄歇辅助陷阱共存,俄歇辅助陷阱在标准太阳光照下主导复合,为钙钛矿光伏效率优化提供了关键框架。

AI 中文摘要

理解金属卤化物钙钛矿中的电荷载流子复合对准确识别限制太阳能电池效率的因素至关重要,但由于多个竞争过程的相互作用,这一问题仍具挑战性。本研究结合宽 fluence(注量)和重复率范围内的时间分辨光致发光与激发依赖的光致发光量子产率测量,探究三阳离子钙钛矿薄膜的复合动力学。通过联合分析这些多维数据集,构建了一个统一模型,该模型可定量复现所有激发条件下的光致发光衰减与绝对量子产率。研究结果揭示了深陷阱、浅陷阱的共存,以及归因于俄歇辅助陷阱的二阶非辐射复合路径;重要的是,该机制在标准太阳光照下占主导,成为光伏性能的关键限制因素。这些发现为理解钙钛矿的复合提供了全面框架,并强调了高阶缺陷介导过程对其效率的重要性。

英文摘要

Understanding charge-carrier recombination in metal halide perovskites is essential for accurately identifying the factors limiting solar cell efficiency, yet it remains challenging due to the interplay of multiple competing processes. Here, we combine time-resolved photoluminescence and excitation dependent photoluminescence quantum yield measurements over a wide range of fluences and repetition rates to investigate recombination dynamics in triple-cation perovskite thin films. By jointly analyzing these multidimensional datasets, we develop a unified model that quantitatively reproduces both photoluminescence decays and absolute quantum yields across all excitation conditions. Our results reveal the coexistence of deep and shallow traps, as well as a second-order nonradiative recombination pathway attributed to Auger-assisted trapping. Importantly, this mechanism dominates under one-sun illumination, making it a critical limiting factor for photovoltaic performance. These findings provide a comprehensive framework for understanding recombination in perovskites and highlight the importance of higher-order defect-mediated processes in determining their efficiency.

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