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Evidence of Large Polarons in Photoemission Band Mapping of the Perovskite Semiconductor CsPbBr3

MPS-Authors
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Xian,  R. Patrick
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Rettig,  Laurenz
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Ernstorfer,  Ralph
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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1909.00248.pdf
(Preprint), 8MB

PhysRevLett.124.206402.pdf
(Publisher version), 2MB

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Citation

Puppin, M., Polishchuk, S., Colonna, N., Crepaldi, A., Dirin, D. N., Nazarenko, O., et al. (2020). Evidence of Large Polarons in Photoemission Band Mapping of the Perovskite Semiconductor CsPbBr3. Physical Review Letters, 124(20): 206402. doi:10.1103/PhysRevLett.124.206402.


Cite as: https://hdl.handle.net/21.11116/0000-0005-3C1B-B
Abstract
Lead-halide perovskite (LHP) semiconductors are emergent optoelectronic materials with outstanding transport properties which are not yet fully understood. We find signatures of large polaron formation in the electronic
structure of the inorganic LHP CsPbBr3 by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass 0.26 ± 0.02 me, 50% heavier than the bare mass m0=0.17 me predicted by density functional theory. Calculations of electron-phonon coupling indicate that phonon dressing of the carriers mainly occurs via distortions of the Pb-Br bond with a Fröhlich coupling parameter α=1.82. A good agreement with our experimental data is obtained within the Feynmann polaron model, validating a viable theorical method to predict the carrier effective mass of LHPs ab-initio.