2020
DOI: 10.1103/physrevlett.124.206402
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Evidence of Large Polarons in Photoemission Band Mapping of the Perovskite Semiconductor CsPbBr3

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 CsPbBr 3 by means of angle-resolved photoelectron spectroscopy. The experimental valence band dispersion shows a hole effective mass of 0.26 AE 0.02 m e , 50% heavier than the bare mass m 0 ¼ 0.17 m e predicted by density functional theory. Calculations of the ele… Show more

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Cited by 93 publications
(92 citation statements)
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“…For CsPbBr 3 , the value of α ≃ 2 corresponds to an intermediate carrier–lattice coupling regime, where the effective mass correction remains relatively small. Cyclotron resonance measurements and estimations of the bare carrier mass via density functional theory suggest that the polaron is only ~50% heavier 21 , 51 , 65 , 66 , which is insufficient to account for the measured Huang–Rhys factor, instead resulting in S ≃ 0.07.…”
Section: Discussionmentioning
confidence: 99%
See 1 more Smart Citation
“…For CsPbBr 3 , the value of α ≃ 2 corresponds to an intermediate carrier–lattice coupling regime, where the effective mass correction remains relatively small. Cyclotron resonance measurements and estimations of the bare carrier mass via density functional theory suggest that the polaron is only ~50% heavier 21 , 51 , 65 , 66 , which is insufficient to account for the measured Huang–Rhys factor, instead resulting in S ≃ 0.07.…”
Section: Discussionmentioning
confidence: 99%
“…Indeed, it has been shown experimentally that the Fröhlich interaction shapes the room-temperature electronic band structure of CsPbBr 3 (ref. 21 ), and is therefore essential in the description of carrier behavior in potential devices. A good starting point for probing the Fröhlich interaction is to conduct measurements at cryogenic temperatures, noting that the impact of the Fröhlich interaction on carrier behavior should only increase towards higher temperatures, as LO phonons become thermally available.…”
Section: Introductionmentioning
confidence: 99%
“…The most dramatic visualization of this effect comes from the identification of up to fourth-order multiphonon transitions in Raman scattering from purely inorganic perovskite NCs, as well as the demonstration of polaronic features in photoelectron spectra. 35 Figure 4g shows Raman spectra of the NCs used here, excited at 780 nm. The dominant optical phonon of these nanocrystals is observed at around 160 meV, which is higher than in purely inorganic perovskite NCs.…”
Section: Nano Lettersmentioning
confidence: 99%
“…3,12,20,[27][28][29] Even though impressive progress in synthesis and device engineering has been made, some fundamental properties of LHPs remain poorly investigated. Particularly, the understanding of the lattice dynamics of LHPs is crucial for the further optimization of their performance due to the unusually high softness of LHPs compared to conventional semiconductors [30][31][32] and the additional dynamic effects caused by the non-spherical geometry of organic A-cations. Their dipole moments in combination with the X-ion migration 33 and the reorientation of A-cations within the BX 6octahedral frame 34 result in a structural phase transition.…”
Section: Introductionmentioning
confidence: 99%