Although solution processing methods provide an attractive route toward development of low-cost functional materials, these accessible fabrication approaches can engender high concentrations of microscopic structural defects that are detrimental to performance. In lead halide perovskites, structural disorder derived from solution processing has been implicated as an important determiner of photophysical properties. However, a direct correlation between the functional properties of these materials and the local crystal structure in which non-equilibrium states evolve has remained elusive, in part because structural heterogeneities occur on length scales that defy conventional characterization techniques. To address this knowledge gap, we have combined ultrafast pump–probe microscopy and electron backscattering diffraction to directly correlate charge carrier transport with the local diffraction pattern contrast, an indicator of crystal quality. Spatial correlation of these measurements strongly suggests that even on individual single crystal CsPbBr₃ domains, microscopic variability in the crystal quality profoundly impacts the efficiency of charge carrier transport.

中文翻译：

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卤化钙钛矿中电荷载流子输运与当地晶体质量的直接相关。

尽管溶液处理方法为开发低成本功能材料提供了一条诱人的途径，但是这些易于使用的制造方法会产生大量对性能有害的微观结构缺陷。在卤化钙钛矿中，源自溶液加工的结构紊乱被认为是光物理性质的重要决定因素。然而，这些材料的功能特性与非平衡态演化的局部晶体结构之间的直接相关性仍然难以捉摸，部分原因是结构异质性发生在不符合常规表征技术的长度尺度上。为了弥补这一知识差距，我们将超快泵浦探针显微镜和电子反向散射衍射相结合，将电荷载流子传输与局部衍射图样对比度（晶体质量的指标）直接相关。这些测量值的空间相关性强烈表明，即使在单个单晶CsPbBr上_在3个域中，晶体质量的微观变化深刻影响着载流子传输的效率。