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  Two-dimensional electronic spectroscopy reveals liquid-like lineshape dynamics in CsPbI3 perovskite nanocrystals

Seiler, H., Palato, S., Sonnichsen, C., Baker, H., Socie, E., Strandell, D. P., et al. (2019). Two-dimensional electronic spectroscopy reveals liquid-like lineshape dynamics in CsPbI3 perovskite nanocrystals. Nature Communications, 10: 4962. doi:10.1038/s41467-019-12830-1.

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 Creators:
Seiler, Helene1, 2, Author           
Palato, Samuel1, 2, Author           
Sonnichsen, Colin2, Author
Baker, Harry2, Author
Socie, Etienne2, 3, Author
Strandell, Dallas P.2, Author
Kambhampati, Patanjali2, Author
Affiliations:
1Physical Chemistry, Fritz Haber Institute, Max Planck Society, ou_634546              
2Department of Chemistry, McGill University, 801 Sherbrooke St. West, Montréal, Québec, Canada, ou_persistent22              
3Lausanne Centre for Ultrafast Science (LACUS), École polytechnique fédérale de Lausanne, 1015, Lausanne, Switzerland, ou_persistent22              

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 Abstract: Lead-halide perovskites have attracted tremendous attention, initially for their performance in thin film photovoltaics, and more recently for a variety of remarkable optical properties. Defect tolerance through polaron formation within the ionic lattice is a key aspect of these materials. Polaron formation arises from the dynamical coupling of atomic fluctuations to electronic states. Measuring the properties of these fluctuations is therefore essential in light of potential optoelectronic applications. Here we apply two-dimensional electronic spectroscopy (2DES) to probe the timescale and amplitude of the electronic gap correlations in CsPbI3 perovskite nanocrystals via homogeneous lineshape dynamics. The 2DES data reveal irreversible, diffusive dynamics that are qualitatively inconsistent with the coherent dynamics in covalent solids such as CdSe quantum dots. In contrast, these dynamics are consistent with liquid-like structural dynamics on the 100 femtosecond timescale. These dynamics are assigned to the optical signature of polaron formation, the conceptual solid-state analogue of solvation.

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Language(s): eng - English
 Dates: 2019-03-282019-09-272019-10-31
 Publication Status: Published online
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1038/s41467-019-12830-1
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Title: Nature Communications
  Abbreviation : Nat. Commun.
Source Genre: Journal
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Publ. Info: London : Nature Publishing Group
Pages: 8 Volume / Issue: 10 Sequence Number: 4962 Start / End Page: - Identifier: ISSN: 2041-1723
CoNE: https://pure.mpg.de/cone/journals/resource/2041-1723