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Polaronic Mass Enhancement and Polaronic Excitons in Metal Halide Perovskites

Abstract:
In metal halide perovskites, the complex dielectric screening together with low energy of phonon modes leads to non-negligible Fröhlich coupling. While this feature of perovskites has already been used to explain some of the puzzling aspects of carrier transport in these materials, the possible impact of polaronic effects on the optical response, especially excitonic properties, is much less explored. Here, with the use of magneto-optical spectroscopy, we revealed the non-hydrogenic character of the excitons in metal halide perovskites, resulting from the pronounced Fröhlich coupling. Our results can be well described by the polaronic-exciton picture where electron and hole interactions are no longer described by a Coulomb potential. Furthermore, we show experimental evidence that the carrier-phonon interaction leads to the enhancement of the carrier's effective mass. Notably, our measurements reveal a pronounced temperature dependence of the carrier's effective mass, which we attribute to a band structure renormalization induced by the population of low-energy phonon modes. This interpretation finds support in our first-principles calculations.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/acsenergylett.4c00905

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Role:
Author
ORCID:
0000-0002-5974-0850
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Role:
Author
ORCID:
0000-0002-4833-4259
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Role:
Author
ORCID:
0000-0003-4945-8795
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Role:
Author
ORCID:
0000-0003-4078-4965


Publisher:
American Chemical Society
Journal:
ACS Energy Letters More from this journal
Volume:
9
Issue:
6
Pages:
2696-2702
Publication date:
2024-05-13
DOI:
EISSN:
2380-8195
ISSN:
2380-8195
Pmid:
38903402


Language:
English
Pubs id:
2004499
Local pid:
pubs:2004499
Source identifiers:
2076662
Deposit date:
2024-06-29
ARK identifier:
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