Frohna Kyle, Chosy Cullen, Al-Ashouri Amran, Scheler Florian, Chiang Yu-Hsien, Dubajic Milos, Parker Julia E, Walker Jessica M, Zimmermann Lea, Selby Thomas A, Lu Yang, Roose Bart, Albrecht Steve, Anaya Miguel, Stranks Samuel D
Department of Chemical Engineering and Biotechnology, University of Cambridge, Cambridge, UK.
Cavendish Laboratory, University of Cambridge, Cambridge, UK.
Nat Energy. 2025;10(1):66-76. doi: 10.1038/s41560-024-01660-1. Epub 2024 Oct 30.
Microscopy provides a proxy for assessing the operation of perovskite solar cells, yet most works in the literature have focused on bare perovskite thin films, missing charge transport and recombination losses present in full devices. Here we demonstrate a multimodal operando microscopy toolkit to measure and spatially correlate nanoscale charge transport losses, recombination losses and chemical composition. By applying this toolkit to the same scan areas of state-of-the-art, alloyed perovskite cells before and after extended operation, we show that devices with the highest macroscopic performance have the lowest initial performance spatial heterogeneity-a crucial link that is missed in conventional microscopy. We show that engineering stable interfaces is critical to achieving robust devices. Once the interfaces are stabilized, we show that compositional engineering to homogenize charge extraction and to minimize variations in local power conversion efficiency is critical to improve performance and stability. We find that in our device space, perovskites can tolerate spatial disorder in chemistry, but not charge extraction.
显微镜检查为评估钙钛矿太阳能电池的运行情况提供了一种替代方法，然而文献中的大多数研究都集中在裸钙钛矿薄膜上，忽略了完整器件中存在的电荷传输和复合损失。在此，我们展示了一种多模态原位显微镜检查工具包，用于测量纳米级电荷传输损失、复合损失和化学成分，并进行空间关联。通过将该工具包应用于经过长时间运行前后的先进合金化钙钛矿电池的相同扫描区域，我们发现宏观性能最高的器件初始性能空间异质性最低——这是传统显微镜检查中遗漏的一个关键联系。我们表明，设计稳定的界面对于实现稳健的器件至关重要。一旦界面稳定，我们表明进行成分工程以使电荷提取均匀化并最小化局部功率转换效率的变化对于提高性能和稳定性至关重要。我们发现在我们的器件空间中，钙钛矿能够容忍化学上的空间无序，但不能容忍电荷提取方面的无序。
