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  Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite

Duan, H.-G., Tiwari, V., Jha, A., Berdiyorov, G. R., Akimov, A., Vendrell, O., et al. (2020). Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite. Journal of the American Chemical Society, 142(39), 16569-16578. doi:10.1021/jacs.0c03970.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-FBEC-6 Version Permalink: http://hdl.handle.net/21.11116/0000-0007-1CD5-A
Genre: Journal Article

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ja0c03970_si_001.pdf (Supplementary material), 2MB
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Supporting Information. - Global fitting approach, correlation analysis in 2D electronic spectra, 2D power spectra of vibrational modes at 33 and 48 cm–1, vibrational coherences in 2D electronic spectroscopy, Tukey-window Fourier transform, raw traces of the GSB and ESA peaks, wavelet analysis, time evolution of electronic charge, and charge localization at different carrier densities
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https://arxiv.org/abs/2004.04970 (Preprint)
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https://dx.doi.org/10.1021/jacs.0c03970 (Publisher version)
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 Creators:
Duan, H.-G.1, 2, 3, Author              
Tiwari, V.1, 4, Author              
Jha, A.1, Author              
Berdiyorov, G. R.5, Author
Akimov, A.6, Author
Vendrell, O.7, Author
Nayak, P. K.8, Author
Snaith, H. J.8, Author
Thorwart, M.2, 3, Author
Li, Z.1, 9, Author              
Madjet, M. E.5, Author
Miller, R. J. D.1, 3, 10, Author              
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2I. Institut für Theoretische Physik, Universität Hamburg, ou_persistent22              
3The Hamburg Center for Ultrafast Imaging, ou_persistent22              
4Department of Chemistry, University of Hamburg, ou_persistent22              
5Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, Qatar Foundation, ou_persistent22              
6Department of Chemistry, State University of New York at Buffalo, ou_persistent22              
7Physikalisch-Chemisches Institut, Universität Heidelberg, ou_persistent22              
8Department of Physics, University of Oxford, Clarendon Laboratory, ou_persistent22              
9State Key Laboratory for Mesoscopic Physics, School of Physics, Peking University, ou_persistent22              
10The Departments of Chemistry and Physics, University of Toronto, ou_persistent22              

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 Abstract: The success of organic–inorganic perovskites in optoelectronics is dictated by the complex interplay between various underlying microscopic phenomena. The structural dynamics of organic cations and the inorganic sublattice after photoexcitation are hypothesized to have a direct effect on the material properties, thereby affecting the overall device performance. Here, we use ultrafast heterodyne-detected two-dimensional (2D) electronic spectroscopy to reveal impulsively excited vibrational modes of methylammonium (MA) lead iodide perovskite, which drive the structural distortion after photoexcitation. Vibrational analysis of the measured data allows us to monitor the time-evolved librational motion of the MA cation along with the vibrational coherences of the inorganic sublattice. Wavelet analysis of the observed vibrational coherences reveals the coherent generation of the librational motion of the MA cation within ∼300 fs complemented with the coherent evolution of the inorganic skeletal motion. To rationalize this observation, we employed the configuration interaction singles (CIS), which support our experimental observations of the coherent generation of librational motions in the MA cation and highlight the importance of the anharmonic interaction between the MA cation and the inorganic sublattice. Moreover, our advanced theoretical calculations predict the transfer of the photoinduced vibrational coherence from the MA cation to the inorganic sublattice, leading to reorganization of the lattice to form a polaronic state with a long lifetime. Our study uncovers the interplay of the organic cation and inorganic sublattice during formation of the polaron, which may lead to novel design principles for the next generation of perovskite solar cell materials.

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Language(s): eng - English
 Dates: 2020-04-112020-09-012020-09-30
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.0c03970
arXiv: 2004.04970
 Degree: -

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Title: Journal of the American Chemical Society
  Other : JACS
  Other : J. Am. Chem. Soc.
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 142 (39) Sequence Number: - Start / End Page: 16569 - 16578 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870