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From Heterostructures to Solid-Solutions: Structural Tunability in Mixed Halide Perovskites
Advanced Materials ( IF 27.4 ) Pub Date : 2022-10-07 , DOI: 10.1002/adma.202205923 Donghoon Shin 1, 2 , Minliang Lai 2, 3 , Yongjin Shin 1, 2 , Jingshan S Du 1, 2 , Liban Jibril 1, 2 , James M Rondinelli 1, 2 , Chad A Mirkin 1, 2, 3
Advanced Materials ( IF 27.4 ) Pub Date : 2022-10-07 , DOI: 10.1002/adma.202205923 Donghoon Shin 1, 2 , Minliang Lai 2, 3 , Yongjin Shin 1, 2 , Jingshan S Du 1, 2 , Liban Jibril 1, 2 , James M Rondinelli 1, 2 , Chad A Mirkin 1, 2, 3
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The stability, reliability, and performance of halide-perovskite-based devices depend upon the structure, composition, and particle size of the device-enabling materials. Indeed, the degree of ion mixing in multicomponent perovskite crystals, although challenging to control, is a key factor in determining properties. Herein, an emerging method termed evaporation–crystallization polymer pen lithography is used to synthesize and systematically study the degree of ionic mixing of Cs0.5FA0.5PbX3 (FA = formamidinium; X = halide anion, ABX3) crystals, as a function of size, temperature, and composition. These experiments have led to the discovery of a heterostructure morphology where the A-site cations, Cs and FA, are segregated into the core and edge layers, respectively. Simulation and experimental results indicate that the heterostructures form as a consequence of a combination of both differences in solubility of the two ions in solution and the enthalpic preference for Cs–FA ion segregation. This preference for segregation can be overcome to form a solid-solution by decreasing crystal size (<60 nm) or increasing temperature. Finally, these tools are utilized to identify and synthesize solid-solution nanocrystals of Cs0.5FA0.5Pb(Br/I)3 that significantly suppress photoinduced anion migration compared to their bulk counterparts, offering a route to deliberately designed photostable optoelectronic materials.
中文翻译：
从异质结构到固溶体：混合卤化物钙钛矿的结构可调性
基于卤化物-钙钛矿的设备的稳定性、可靠性和性能取决于设备支持材料的结构、组成和粒径。事实上，多组分钙钛矿晶体中的离子混合程度虽然难以控制，但却是决定性能的关键因素。在此，一种称为蒸发结晶聚合物笔光刻的新兴方法用于合成和系统研究 Cs 0.5 FA 0.5 PbX 3的离子混合程度（FA = 甲脒；X = 卤化物阴离子，ABX 3) 晶体，作为尺寸、温度和成分的函数。这些实验导致发现异质结构形态，其中 A 位阳离子 Cs 和 FA 分别分离到核心层和边缘层中。模拟和实验结果表明，异质结构的形成是两种离子在溶液中的溶解度差异和 Cs-FA 离子分离的焓偏好相结合的结果。通过减小晶体尺寸 (<60 nm) 或升高温度，可以克服这种偏析偏好以形成固溶体。最后，这些工具被用于识别和合成 Cs 0.5 FA 0.5 Pb(Br/I) 3的固溶体纳米晶体与大量对应物相比，它显着抑制了光致阴离子迁移，为有意设计的光稳定光电材料提供了一条途径。
更新日期：2022-10-07
中文翻译：
从异质结构到固溶体：混合卤化物钙钛矿的结构可调性
基于卤化物-钙钛矿的设备的稳定性、可靠性和性能取决于设备支持材料的结构、组成和粒径。事实上，多组分钙钛矿晶体中的离子混合程度虽然难以控制，但却是决定性能的关键因素。在此，一种称为蒸发结晶聚合物笔光刻的新兴方法用于合成和系统研究 Cs 0.5 FA 0.5 PbX 3的离子混合程度（FA = 甲脒；X = 卤化物阴离子，ABX 3) 晶体，作为尺寸、温度和成分的函数。这些实验导致发现异质结构形态，其中 A 位阳离子 Cs 和 FA 分别分离到核心层和边缘层中。模拟和实验结果表明，异质结构的形成是两种离子在溶液中的溶解度差异和 Cs-FA 离子分离的焓偏好相结合的结果。通过减小晶体尺寸 (<60 nm) 或升高温度，可以克服这种偏析偏好以形成固溶体。最后，这些工具被用于识别和合成 Cs 0.5 FA 0.5 Pb(Br/I) 3的固溶体纳米晶体与大量对应物相比，它显着抑制了光致阴离子迁移，为有意设计的光稳定光电材料提供了一条途径。
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