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

Guo, Songhao; Mihalyi-Koch, Willa; Mao, Yuhong; Li, Xinyu; Bu, Kejun; Hong, Huilong; Hautzinger, Matthew P.; Luo, Hui; Wang, Dong; Gu, Jiazhen; Zhang, Yifan; Zhang, Dongzhou; Hu, Qingyang; Ding, Yang; Yang, Wenge; Fu, Yongping; Jin, Song; Lü, Xujie

doi:10.1038/s41467-024-47225-4

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

Journal Article · 07 April 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-47225-4 · OSTI ID:2472393

Guo, Songhao ^[1];

^[2]; Mao, Yuhong ^[3]; Li, Xinyu ^[4];

^[3];

^[4];

^[2]; Luo, Hui ^[3];

^[3]; Gu, Jiazhen ^[4]; Zhang, Yifan ^[3];

^[5];

^[3];

^[4];

^[2];

^[6]

Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China); OSTI
Univ. of Wisconsin, Madison, WI (United States)
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
Peking Univ., Beijing (China)
Univ. of Hawaii at Manoa, Honolulu, HI (United States)
Center for High Pressure Science and Technology Advanced Research (HPSTAR), Beijing (China)

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%.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Organization:: National Nature Science Foundation of China (NSFC); Shanghai Key Laboratory of Novel Extreme Condition Materials; Shanghai Science and Technology Committee; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-06CH11357; SC0002162

OSTI ID:: 2472393

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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