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, Kai Leng

Research output: Journal article publicationJournal articleAcademic researchpeer-review

10 Citations (Scopus)

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.

Original languageEnglish
Article number138
JournalNature Communications
Volume13
Issue number1
DOIs
Publication statusPublished - Dec 2022

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

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