Local Polar Fluctuations in Lead Halide Perovskite Crystals

Omer Yaffe, Yinsheng Guo, Liang Z. Tan, David A. Egger, Trevor Hull, Constantinos C. Stoumpos, Fan Zheng, Tony F. Heinz, Leeor Kronik, Mercouri G Kanatzidis, Jonathan S. Owen, Andrew M. Rappe, Marcos A. Pimenta, Louis E. Brus

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Abstract

Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low-frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in the cubic phase of both hybrid (CH3NH3PbBr3) and all-inorganic (CsPbBr3) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations indicate that head-to-head Cs motion coupled to Br face expansion, occurring on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr3.

Original languageEnglish
Article number136001
JournalPhysical Review Letters
Volume118
Issue number13
DOIs
Publication statusPublished - Mar 28 2017

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halides
perovskites
crystals
molecular dynamics
cations
Raman spectra
low frequencies
expansion
simulation

ASJC Scopus subject areas

  • Physics and Astronomy(all)

Cite this

Yaffe, O., Guo, Y., Tan, L. Z., Egger, D. A., Hull, T., Stoumpos, C. C., ... Brus, L. E. (2017). Local Polar Fluctuations in Lead Halide Perovskite Crystals. Physical Review Letters, 118(13), [136001]. https://doi.org/10.1103/PhysRevLett.118.136001

Local Polar Fluctuations in Lead Halide Perovskite Crystals. / Yaffe, Omer; Guo, Yinsheng; Tan, Liang Z.; Egger, David A.; Hull, Trevor; Stoumpos, Constantinos C.; Zheng, Fan; Heinz, Tony F.; Kronik, Leeor; Kanatzidis, Mercouri G; Owen, Jonathan S.; Rappe, Andrew M.; Pimenta, Marcos A.; Brus, Louis E.

In: Physical Review Letters, Vol. 118, No. 13, 136001, 28.03.2017.

Research output: Contribution to journalArticle

Yaffe, O, Guo, Y, Tan, LZ, Egger, DA, Hull, T, Stoumpos, CC, Zheng, F, Heinz, TF, Kronik, L, Kanatzidis, MG, Owen, JS, Rappe, AM, Pimenta, MA & Brus, LE 2017, 'Local Polar Fluctuations in Lead Halide Perovskite Crystals', Physical Review Letters, vol. 118, no. 13, 136001. https://doi.org/10.1103/PhysRevLett.118.136001
Yaffe O, Guo Y, Tan LZ, Egger DA, Hull T, Stoumpos CC et al. Local Polar Fluctuations in Lead Halide Perovskite Crystals. Physical Review Letters. 2017 Mar 28;118(13). 136001. https://doi.org/10.1103/PhysRevLett.118.136001
Yaffe, Omer ; Guo, Yinsheng ; Tan, Liang Z. ; Egger, David A. ; Hull, Trevor ; Stoumpos, Constantinos C. ; Zheng, Fan ; Heinz, Tony F. ; Kronik, Leeor ; Kanatzidis, Mercouri G ; Owen, Jonathan S. ; Rappe, Andrew M. ; Pimenta, Marcos A. ; Brus, Louis E. / Local Polar Fluctuations in Lead Halide Perovskite Crystals. In: Physical Review Letters. 2017 ; Vol. 118, No. 13.
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