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

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 () and Kai Leng ()
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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

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-021-27747-x

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