Exciton engineering of 2D Ruddlesden–Popper perovskites by synergistically tuning the intra and interlayer structures

作者：Songhao Guo, Willa Mihalyi‐Koch, Yuhong Mao, Xinyu Li, Kejun Bu, Huilong Hong, Matthew P. Hautzinger, Hui Luo, Dong Wang, Jiazhen Gu, Yifan Zhang, Dongzhou Zhang, Qingyang Hu, Yang Ding, Wenge Yang, Yongping Fu, Song Jin, Xujie Lü · 发表于：Nature Communications · 年份：2024 · DOI：10.1038/s41467-024-47225-4 · 被引用次数：108 · 研究领域：Perovskite Materials and Applications、2D Materials and Applications、Solid-state spectroscopy and crystallography

Abstract Designing two-dimensional halide perovskites for high-performance optoelectronic applications requires deep understanding of the structure-property relationship that governs their excitonic behaviors. However, a design framework that considers both intra and interlayer structures modified by the A-site and spacer cations, respectively, has not been developed. Here, we use pressure to synergistically tune the intra and interlayer structures and uncover the structural modulations that result in improved optoelectronic performance. Under applied pressure, (BA) 2 (GA)Pb 2 I 7 exhibits a 72-fold boost of photoluminescence and 10-fold increase of photoconductivity. Based on the observed structural change, we introduce a structural descriptor χ that describes both the intra and interlayer characteristics and establish a general quantitative relationship between χ and photoluminescence quantum yield: smaller χ correlates with minimized trapped excitons and more efficient emission from free excitons. Building on this principle, we design a perovskite (CMA) 2 (FA)Pb 2 I 7 that exhibits a small χ and an impressive photoluminescence quantum yield of 59.3%.