Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.337
Publication date: 7th February 2022
Mixed-dimensional perovskites containing mixtures of organic cations hold great promise to deliver highly stable and efficient solar cells. When used in small amounts, the low-dimensional species can act as a dopant to passivate defects at the grain boundaries of the 3D counterpart, leading to improved performance and stability. However, although a plethora of relatively bulky organic cations have been reported for such purpose, a fundamental understanding of the materials' structure, composition, and phase, along with their correlated effects on the corresponding optoelectronic properties and degradation mechanism remains elusive. Herein, we systematically engineer the structures of bulky organic cations to template the formation of low-dimensional perovskites with contrasting inorganic framework dimensionality (2D to 0D), connectivity (flat vs. corrugated), and coordination deformation. By combining X-ray single-crystal structural analysis with various spectroscopic techniques, such as depth-profiling XPS, solid-state NMR, and femtosecond transient absorption, it is revealed that not all low-dimensional species work equally well as dopants. Instead, it was found that inorganic architectures with lesser structural distortion tend to yield a less disordered energetic and defect landscape in the resulting mixed-dimensional perovskites, augmented in materials with higher PLQY (up to 11%), better solar cell performance (PCE more than 19%) and improved thermal stability (T70 up to 1000 hrs, unencapsulated). Our study highlights the importance of designing templating organic cations that yield low-dimensional materials with much less structural distortion profiles to be used as additives in stable and efficient perovskite solar cells.
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