Hybrid Dion-Jacobson 2D Lead Iodide Perovskites,Journal of the American Chemical Society

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Hybrid Dion-Jacobson 2D Lead Iodide Perovskites
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-02-21 , DOI: 10.1021/jacs.8b00542
Lingling Mao , Weijun Ke , Laurent Pedesseau ₁ , Yilei Wu , Claudine Katan ₂ , Jacky Even ₁ , Michael R. Wasielewski , Constantinos C. Stoumpos , Mercouri G. Kanatzidis

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The three-dimensional hybrid organic-inorganic perovskites have shown huge potential for use in solar cells and other optoelectronic devices. Although these materials are under intense investigation, derivative materials with lower dimensionality are emerging, offering higher tunability of physical properties and new capabilities. Here, we present two new series of hybrid two-dimensional (2D) perovskites that adopt the Dion-Jacobson (DJ) structure type, which are the first complete homologous series reported in halide perovskite chemistry. Lead iodide DJ perovskites adopt a general formula A'A n-1Pb nI3 n+1 (A' = 3-(aminomethyl)piperidinium (3AMP) or 4-(aminomethyl)piperidinium (4AMP), A = methylammonium (MA)). These materials have layered structures where the stacking of inorganic layers is unique as they lay exactly on top of another. With a slightly different position of the functional group in the templating cation 3AMP and 4AMP, the as-formed DJ perovskites show different optical properties, with the 3AMP series having smaller band gaps than the 4AMP series. Analysis on the crystal structures and density functional theory (DFT) calculations suggest that the origin of the systematic band gap shift is the strong but indirect influence of the organic cation on the inorganic framework. Fabrication of photovoltaic devices utilizing these materials as light absorbers reveals that (3AMP)(MA)3Pb4I13 has the best power conversion efficiency (PCE) of 7.32%, which is much higher than that of the corresponding (4AMP)(MA)3Pb4I13.

中文翻译：

混合 Dion-Jacobson 二维铅碘化物钙钛矿

三维杂化有机-无机钙钛矿已在太阳能电池和其他光电器件中显示出巨大的应用潜力。尽管对这些材料进行了深入研究，但正在出现具有较低维数的衍生材料，提供更高的物理特性可调性和新功能。在这里，我们展示了两个新系列的混合二维 (2D) 钙钛矿，它们采用 Dion-Jacobson (DJ) 结构类型，这是卤化物钙钛矿化学中报道的第一个完整的同源系列。碘化铅DJ钙钛矿采用通式A'A n-1Pb nI3 n+1（A' = 3-（氨甲基）哌啶鎓（3AMP）或4-（氨甲基）哌啶鎓（4AMP），A =甲基铵（MA））。这些材料具有分层结构，其中无机层的堆叠是独一无二的，因为它们恰好位于另一个之上。由于模板阳离子 3AMP 和 4AMP 中官能团的位置略有不同，形成的 DJ 钙钛矿显示出不同的光学特性，3AMP 系列的带隙比 4AMP 系列更小。对晶体结构和密度泛函理论 (DFT) 计算的分析表明，系统带隙位移的起源是有机阳离子对无机骨架的强烈但间接的影响。利用这些材料作为光吸收剂制造光伏器件表明，(3AMP)(MA)3Pb4I13 的最佳功率转换效率 (PCE) 为 7.32%，远高于相应的 (4AMP)(MA)3Pb4I13。与 4AMP 系列相比，3AMP 系列的带隙更小。对晶体结构和密度泛函理论 (DFT) 计算的分析表明，系统带隙位移的起源是有机阳离子对无机骨架的强烈但间接的影响。利用这些材料作为光吸收剂制造光伏器件表明，(3AMP)(MA)3Pb4I13 的最佳功率转换效率 (PCE) 为 7.32%，远高于相应的 (4AMP)(MA)3Pb4I13。与 4AMP 系列相比，3AMP 系列的带隙更小。对晶体结构和密度泛函理论 (DFT) 计算的分析表明，系统带隙位移的起源是有机阳离子对无机骨架的强烈但间接的影响。利用这些材料作为光吸收剂制造光伏器件表明，(3AMP)(MA)3Pb4I13 的最佳功率转换效率 (PCE) 为 7.32%，远高于相应的 (4AMP)(MA)3Pb4I13。

更新日期：2018-02-21

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