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Unlocking surface octahedral tilt in two-dimensional Ruddlesden-Popper perovskites

Author

Listed:
  • Yan Shao

    (National University of Singapore)

  • Wei Gao

    (The Hong Kong Polytechnic University)

  • Hejin Yan

    (University of Macau)

  • Runlai Li

    (National University of Singapore)

  • Ibrahim Abdelwahab

    (National University of Singapore)

  • Xiao Chi

    (National University of Singapore)

  • Lukas Rogée

    (The Hong Kong Polytechnic University)

  • Lyuchao Zhuang

    (The Hong Kong Polytechnic University)

  • Wei Fu

    (National University of Singapore)

  • Shu Ping Lau

    (The Hong Kong Polytechnic University)

  • Siu Fung Yu

    (The Hong Kong Polytechnic University)

  • Yongqing Cai

    (University of Macau)

  • Kian Ping Loh

    (National University of Singapore)

  • Kai Leng

    (The Hong Kong Polytechnic University)

Abstract

Molecularly soft organic-inorganic hybrid perovskites are susceptible to dynamic instabilities of the lattice called octahedral tilt, which directly impacts their carrier transport and exciton-phonon coupling. Although the structural phase transitions associated with octahedral tilt has been extensively studied in 3D hybrid halide perovskites, its impact in hybrid 2D perovskites is not well understood. Here, we used scanning tunneling microscopy (STM) to directly visualize surface octahedral tilt in freshly exfoliated 2D Ruddlesden-Popper perovskites (RPPs) across the homologous series, whereby the steric hindrance imposed by long organic cations is unlocked by exfoliation. The experimentally determined octahedral tilts from n = 1 to n = 4 RPPs from STM images are found to agree very well with out-of-plane surface octahedral tilts predicted by density functional theory calculations. The surface-enhanced octahedral tilt is correlated to excitonic redshift observed in photoluminescence (PL), and it enhances inversion asymmetry normal to the direction of quantum well and promotes Rashba spin splitting for n > 1.

Suggested Citation

  • Yan Shao & Wei Gao & Hejin Yan & Runlai Li & Ibrahim Abdelwahab & Xiao Chi & Lukas Rogée & Lyuchao Zhuang & Wei Fu & Shu Ping Lau & Siu Fung Yu & Yongqing Cai & Kian Ping Loh & Kai Leng, 2022. "Unlocking surface octahedral tilt in two-dimensional Ruddlesden-Popper perovskites," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-021-27747-x
    DOI: 10.1038/s41467-021-27747-x
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    Cited by:

    1. 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.
    2. Dejian Yu & Fei Cao & Jinfeng Liao & Bingzhe Wang & Chenliang Su & Guichuan Xing, 2022. "Direct observation of photoinduced carrier blocking in mixed-dimensional 2D/3D perovskites and the origin," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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