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

Author

Listed:
  • 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))

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%.

Suggested Citation

  • 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 &, 2024. "Exciton engineering of 2D Ruddlesden–Popper perovskites by synergistically tuning the intra and interlayer structures," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47225-4
    DOI: 10.1038/s41467-024-47225-4
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    References listed on IDEAS

    as
    1. Xiaoming Zhao & Melissa L. Ball & Arvin Kakekhani & Tianran Liu & Andrew M. Rappe & Yueh-Lin Loo, 2022. "A charge transfer framework that describes supramolecular interactions governing structure and properties of 2D perovskites," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Kejun Bu & Qingyang Hu & Xiaohuan Qi & Dong Wang & Songhao Guo & Hui Luo & Tianquan Lin & Xiaofeng Guo & Qiaoshi Zeng & Yang Ding & Fuqiang Huang & Wenge Yang & Ho-Kwang Mao & Xujie Lü, 2022. "Nested order-disorder framework containing a crystalline matrix with self-filled amorphous-like innards," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Weijian Tao & Chi Zhang & Qiaohui Zhou & Yida Zhao & Haiming Zhu, 2021. "Momentarily trapped exciton polaron in two-dimensional lead halide perovskites," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    4. Yuanzhi Jiang & Minghuan Cui & Saisai Li & Changjiu Sun & Yanmin Huang & Junli Wei & Li Zhang & Mei Lv & Chaochao Qin & Yufang Liu & Mingjian Yuan, 2021. "Reducing the impact of Auger recombination in quasi-2D perovskite light-emitting diodes," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    5. Tingting Yin & Hejin Yan & Ibrahim Abdelwahab & Yulia Lekina & Xujie Lü & Wenge Yang & Handong Sun & Kai Leng & Yongqing Cai & Ze Xiang Shen & Kian Ping Loh, 2023. "Pressure driven rotational isomerism in 2D hybrid perovskites," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    6. Guichuan Xing & Bo Wu & Xiangyang Wu & Mingjie Li & Bin Du & Qi Wei & Jia Guo & Edwin K. L. Yeow & Tze Chien Sum & Wei Huang, 2017. "Transcending the slow bimolecular recombination in lead-halide perovskites for electroluminescence," Nature Communications, Nature, vol. 8(1), pages 1-9, April.
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