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Slow Electron–Hole Recombination in Lead Iodide Perovskites Does Not Require a Molecular Dipole
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-09-07 00:00:00 , DOI: 10.1021/acsenergylett.7b00606 Subham Dastidar 1 , Siming Li 1 , Sergey Y. Smolin 1 , Jason B. Baxter 1 , Aaron T. Fafarman 1
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-09-07 00:00:00 , DOI: 10.1021/acsenergylett.7b00606 Subham Dastidar 1 , Siming Li 1 , Sergey Y. Smolin 1 , Jason B. Baxter 1 , Aaron T. Fafarman 1
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Hybrid organic/inorganic lead iodide perovskites of the formula APbI3, where A is a molecular cation such as methylammonium, exhibit remarkably slow photoinduced charge carrier recombination rates, for reasons that remain uncertain. Prevalent hypotheses credit this behavior to the unique dipolar nature of the molecular cation. Herein, transient terahertz spectroscopy is applied to solution-processed, all-inorganic, perovskite-phase cesium lead iodide (CsPbI3) thin films, which lack such a dipole. The recombination kinetics are studied as a function of the initial photoinduced carrier concentration and the wavelength of excitation. A kinetic model combining diffusion and recombination is fit to the data, from which the rate constants are determined, revealing a bimolecular recombination rate of 10–10 cm3 s–1, comparable to high-quality, single-crystal, direct-gap semiconductors. This rate, as well as a charge carrier mobility > 30 cm2 V–1 s–1 measured herein for CsPbI3, are similar to values reported for the hybrid perovskites, strongly suggesting that the organic cation does not confer a fundamental advantage.
中文翻译：
碘化铅钙钛矿中的慢电子-空穴复合不需要分子偶极子。
由于仍不确定的原因，其中A是分子阳离子如甲基铵的式APbI 3的杂化有机/无机碘化铅钙钛矿表现出非常缓慢的光诱导电荷载流子复合速率。普遍的假设将此行为归因于分子阳离子的独特偶极性质。本文中，瞬变太赫兹光谱技术适用于固溶钙钛矿相的碘化铯碘化铯（CsPbI 3）薄膜，但缺少这种偶极子。研究了重组动力学与初始光诱导载流子浓度和激发波长的关系。结合扩散和重组的动力学模型适合数据，由此确定速率常数，揭示出10 –10 cm 3 s –1的双分子重组速率，可与高质量，单晶，直接间隙半导体相比。对于CsPbI 3，该速率以及此处测得的CsPbI 3的载流子迁移率> 30 cm 2 V –1 s –1，与报道的杂化钙钛矿的值相似，强烈表明有机阳离子没有赋予基本优势。
更新日期：2017-09-07
中文翻译：
碘化铅钙钛矿中的慢电子-空穴复合不需要分子偶极子。
由于仍不确定的原因，其中A是分子阳离子如甲基铵的式APbI 3的杂化有机/无机碘化铅钙钛矿表现出非常缓慢的光诱导电荷载流子复合速率。普遍的假设将此行为归因于分子阳离子的独特偶极性质。本文中，瞬变太赫兹光谱技术适用于固溶钙钛矿相的碘化铯碘化铯（CsPbI 3）薄膜，但缺少这种偶极子。研究了重组动力学与初始光诱导载流子浓度和激发波长的关系。结合扩散和重组的动力学模型适合数据，由此确定速率常数，揭示出10 –10 cm 3 s –1的双分子重组速率，可与高质量，单晶，直接间隙半导体相比。对于CsPbI 3，该速率以及此处测得的CsPbI 3的载流子迁移率> 30 cm 2 V –1 s –1，与报道的杂化钙钛矿的值相似，强烈表明有机阳离子没有赋予基本优势。
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