Organic–inorganic hybrid perovskites have electronic and optoelectronic properties that make them appealing in many device applications1–4. Although many approaches focus on polycrystalline materials5–7, single-crystal hybrid perovskites show improved carrier transport and enhanced stability over their polycrystalline counterparts, due to their orientation-dependent transport behaviour8–10 and lower defect concentrations11,12. However, the fabrication of single-crystal hybrid perovskites, and controlling their morphology and composition, are challenging12. Here we report a solution-based lithography-assisted epitaxial-growth-and-transfer method for fabricating single-crystal hybrid perovskites on arbitrary substrates, with precise control of their thickness (from about 600 nanometres to about 100 micrometres), area (continuous thin films up to about 5.5 centimetres by 5.5 centimetres), and composition gradient in the thickness direction (for example, from methylammonium lead iodide, MAPbI3, to MAPb0.5Sn0.5I3). The transferred single-crystal hybrid perovskites are of comparable quality to those directly grown on epitaxial substrates, and are mechanically flexible depending on the thickness. Lead–tin gradient alloying allows the formation of a graded electronic bandgap, which increases the carrier mobility and impedes carrier recombination. Devices based on these single-crystal hybrid perovskites show not only high stability against various degradation factors but also good performance (for example, solar cells based on lead–tin-gradient structures with an average efficiency of 18.77 per cent). A solution-based lithography-assisted epitaxial-growth-and-transfer method is used to fabricate single-crystal hybrid perovskites on any surface, with precise control of the thickness, area and chemical composition gradient.

中文翻译：

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一种柔性单晶钙钛矿器件的制造工艺

有机-无机杂化钙钛矿具有电子和光电特性，使其在许多设备应用中具有吸引力1-4。尽管许多方法专注于多晶材料 5-7，但单晶杂化钙钛矿显示出比多晶材料更好的载流子传输和更高的稳定性，这是由于它们的取向相关传输行为 8-10 和较低的缺陷浓度 11,12。然而，单晶杂化钙钛矿的制造以及控制其形态和成分具有挑战性12。在这里，我们报告了一种基于溶液的光刻辅助外延生长和转移方法，用于在任意衬底上制造单晶混合钙钛矿，并精确控制其厚度（从约 600 纳米到约 100 微米），面积（最大约 5.5 厘米 x 5.5 厘米的连续薄膜），以及厚度方向的成分梯度（例如，从甲基碘化铅 MAPbI3 到 MAPb0.5Sn0.5I3）。转移的单晶杂化钙钛矿与直接在外延衬底上生长的钙钛矿质量相当，并且根据厚度具有机械柔性。铅锡梯度合金化允许形成梯度电子带隙，从而增加载流子迁移率并阻止载流子复合。基于这些单晶混合钙钛矿的器件不仅对各种退化因素表现出高稳定性，而且还表现出良好的性能（例如，基于铅锡梯度结构的太阳能电池，平均效率为 18.77%）。