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

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 () and Xujie Lü ()
Additional contact information
Songhao Guo: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Willa Mihalyi-Koch: University of Wisconsin-Madison
Yuhong Mao: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Xinyu Li: Peking University
Kejun Bu: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Huilong Hong: Peking University
Matthew P. Hautzinger: University of Wisconsin-Madison
Hui Luo: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Dong Wang: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Jiazhen Gu: Peking University
Yifan Zhang: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Dongzhou Zhang: University of Hawaii Manoa
Qingyang Hu: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Yang Ding: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Wenge Yang: Center for High Pressure Science and Technology Advanced Research (HPSTAR)
Yongping Fu: Peking University
Song Jin: University of Wisconsin-Madison
Xujie Lü: Center for High Pressure Science and Technology Advanced Research (HPSTAR)

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: 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)Pb2I7 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)Pb2I7 that exhibits a small χ and an impressive photoluminescence quantum yield of 59.3%.

Date: 2024
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DOI: 10.1038/s41467-024-47225-4

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