Synergy between Ion Migration and Charge Carrier Recombination in Metal-Halide Perovskites,Journal of the American Chemical Society

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Synergy between Ion Migration and Charge Carrier Recombination in Metal-Halide Perovskites
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-01-22 , DOI: 10.1021/jacs.9b12391
Chuan-Jia Tong _{1,

2,

3} , Linqiu Li ₂ , Li-Min Liu ₁ , Oleg V Prezhdo ₂

Affiliation

Charge carrier recombination plays a vital role in the CH3NH3PbI3 perovskite solar cell. By investigating a possible synergy between ion migration and charge carrier recombination, we demonstrate that the nonradiative recombination accelerates by an order of magnitude during iodide migration. The migration induces lattice distortion that brings electrons and holes close to each other and increases their electrostatic interactions. The wave function localization in the same spatial region, and the enhanced lattice and iodide movements increase the nonadiabatic coupling. At the same time, quantum coherence lasts longer, because electron and hole energy levels become correlated. All these factors greatly increase the recombination rate. Moreover, the energy level of the iodide vacancy created during the migration moves from inside the conduction band in the equilibrated structure into the band gap, acting as a typical efficient nonradiative charge recombination center. Our work shows that the different dynamic processes are strongly correlated in halide perovskites, and demonstrates that defects, considered to be benign, can become very detrimental under non-equilibrium conditions. The reported results strongly suggest that ion migration should be avoided in halide perovskites, both for own reasons, such as large current-voltage hysteresis, and because it greatly accelerates charge carrier losses.

中文翻译：

金属卤化物钙钛矿中离子迁移与载流子复合的协同作用

载流子复合在 CH3NH3PbI3 钙钛矿太阳能电池中起着至关重要的作用。通过研究离子迁移和电荷载流子复合之间可能的协同作用，我们证明了非辐射复合在碘迁移过程中加速了一个数量级。迁移引起晶格畸变，使电子和空穴彼此靠近并增加它们的静电相互作用。同一空间区域的波函数局域化，以及增强的晶格和碘化物运动增加了非绝热耦合。同时，量子相干性持续时间更长，因为电子和空穴的能级变得相关。所有这些因素都大大提高了重组率。而且，迁移过程中产生的碘化物空位的能级从平衡结构中的导带内部移动到带隙中，充当典型的高效非辐射电荷复合中心。我们的工作表明，卤化物钙钛矿中不同的动态过程密切相关，并表明被认为是良性的缺陷在非平衡条件下会变得非常有害。报告的结果强烈表明在卤化物钙钛矿中应该避免离子迁移，这既是出于自身原因，例如大电流-电压滞后，也因为它大大加速了电荷载流子的损失。我们的工作表明，卤化物钙钛矿中不同的动态过程密切相关，并表明被认为是良性的缺陷在非平衡条件下会变得非常有害。报告的结果强烈表明在卤化物钙钛矿中应避免离子迁移，这既是出于自身原因，例如大电流-电压滞后，也因为它大大加速了电荷载流子的损失。我们的工作表明，卤化物钙钛矿中不同的动态过程密切相关，并表明被认为是良性的缺陷在非平衡条件下会变得非常有害。报告的结果强烈表明在卤化物钙钛矿中应避免离子迁移，这既是出于自身原因，例如大电流-电压滞后，也因为它大大加速了电荷载流子的损失。

更新日期：2020-01-22

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