Layer-by-Layer Structural Identification of 2D Ruddlesden-Popper Hybrid Lead Iodide Perovskites by Solid-State NMR Spectroscopy

Jeongjae Lee, Woocheol Lee, Keehoon Kang, Takhee Lee, Sung Keun Lee

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1 Citation (Scopus)

Abstract

Application of two-dimensional (2D) organic-inorganic hybrid halide perovskites in optoelectronic devices requires a detailed understanding of the local structural features including the Pb-I bonding in the 2D layers and the organic-inorganic interaction between the organic spacer molecules and the perovskite layer. In this study, we show that 1H and 207Pb solid-state nuclear magnetic resonance (NMR) spectroscopy can serve as a noninvasive and complementary technique to probe the local structural features of the 2D Ruddlesden-Popper phase BA2MAn-1PbnI3n+1 (n = 1-4) with butylammonium (BA) spacers. 207Pb echo and 207Pb → 1H heteronuclear correlation experiments enable layer-by-layer structural detection of 2D halide perovskites. We show that the observed correlation between 207Pb NMR shifts and mean Pb-I bond lengths around each Pb site allows us to probe the local bonding environment of Pb. We envisage that this technique will be vital for a better understanding of the properties of materials as determined by the local atomistic environments in multidimensional halide perovskites.

Original languageEnglish
Pages (from-to)370-377
Number of pages8
JournalChemistry of Materials
Volume33
Issue number1
DOIs
Publication statusPublished - 2021 Jan 12

Bibliographical note

Funding Information:
This work was supported by the National Research Foundation of Korea (NRF) grants funded by the Korean government (MSIT) (No. NRF-2020R1A3B2079815 and No. 2012026372) J.L. was supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MEST) (No. 2019R1A6A1A10073437). K.K. appreciates the financial support by Postdoctoral Science Fellowship from POSCO TJ Park Foundation. We thank the three anonymous reviewers for their helpful comments and insights for improving this manuscript.

Publisher Copyright:
© 2020 American Chemical Society.

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Chemical Engineering(all)
  • Materials Chemistry

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