Modeling the Interaction of Molecular Iodine with MAPbI3: A Probe of Lead-Halide Perovskites Defect Chemistry,ACS Energy Letters

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Modeling the Interaction of Molecular Iodine with MAPbI3: A Probe of Lead-Halide Perovskites Defect Chemistry
ACS Energy Letters ( IF 19.3 ) Pub Date : 2018-01-25 00:00:00 , DOI: 10.1021/acsenergylett.7b01244
Daniele Meggiolaro _{1,

2} , Edoardo Mosconi _{1,

3} , Filippo De Angelis _{1,

2,

3}

Affiliation

Understanding the defect chemistry of lead-halide perovskites is of paramount importance to further progress toward exploitation of these materials. Here, we combine recent experimental observations on the behavior of MAPbI₃ upon exposure to I₂ vapor with first-principles calculations to extract a global picture of defect chemistry in lead-halide perovskites. By matching the reported experimental observables we disclose the origin of the p-doping observed upon exposing MAPbI₃ to I₂ and highlight its consequences on the charge and ion transport and trapping activity. Electron/hole traps related to positive/negative interstitial iodine dominate the defect chemistry in intrinsic conditions, while in p-doped MAPbI₃, electrons are mainly trapped by positive interstitial iodine and neutral lead vacancies. I₂ spontaneously dissociates on iodine vacancies, leading to vacancy passivation and to the formation of positive interstitial iodine. I₂ spontaneously dissociates on nondefective MAPbI₃(001) surfaces to form pairs of negative/positive interstitial iodine. Upon trapping a hole/electron pair at negative/positive interstitial iodine, I₂ release becomes thermodynamically favored, possibly representing a photoinduced trap-curing mechanism.

中文翻译：

分子碘与MAPbI ₃相互作用的建模：卤化钙钛矿铅缺陷化学的探索

了解卤化钙钛矿的缺陷化学对于进一步开发这些材料至关重要。在这里，我们将最近对MAPbI ₃暴露于I ₂蒸气后的行为的实验观察结果与第一性原理计算相结合，以提取卤化钙钛矿中缺陷化学的全局图。通过匹配报道的实验可观察物，我们公开了将MAPbI ₃暴露于I _2时观察到的p掺杂的起源，并突出了其对电荷，离子迁移和俘获活性的影响。在固有条件下，与正/负间隙碘有关的电子/空穴陷阱占主导地位，而在p掺杂的MAPbI _3中，电子/空穴陷阱占主导地位。，电子主要被正性间隙碘和中性铅空位俘获。I ₂自发地解离碘空位，导致空位钝化并形成正性间隙碘。I ₂在无缺陷的MAPbI ₃（001）表面上自发解离，形成成对的负/正质间隙碘。在将空穴/电子对俘获在负/正间隙碘上时，I _2的释放在热力学上变得有利，可能代表了光诱导的俘获固化机制。

更新日期：2018-01-25

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