Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite

Yang Lan, Benjamin J. Dringoli, David A. Valverde-Chávez, Carlito S. Ponseca, Mark Sutton, Yihui He, Mercouri G Kanatzidis, David G. Cooke

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties, exhibiting an impressive tolerance to defects believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons. Few experimental techniques are capable of directly probing these correlations, requiring simultaneous sub–millielectron volt energy and femtosecond temporal resolution after absorption of a photon. Here, we use time-resolved multi-THz spectroscopy, sensitive to the internal excitations of the polaron, to temporally and energetically resolve the coherent coupling of charges to longitudinal optical phonons in single-crystal CH3NH3PbI3 (MAPI). We observe room temperature intraband quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide strong evidence for the existence of polarons in MAPI at room temperature, suggesting that electron/hole-phonon coupling is a defining aspect of the hybrid metal-halide perovskites contributing to the protection from scattering and enhanced carrier lifetimes that define their usefulness in devices.

Original languageEnglish
Article numbereaaw5558
JournalScience Advances
Volume5
Issue number5
DOIs
Publication statusPublished - May 31 2019

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metal halides
polarons
perovskites
room temperature
carrier lifetime
temporal resolution
halides
charge carriers
synchronism
phonons
single crystals
defects
photons
scattering
spectroscopy
excitation
energy

ASJC Scopus subject areas

  • General
  • Physics and Astronomy (miscellaneous)

Cite this

Lan, Y., Dringoli, B. J., Valverde-Chávez, D. A., Ponseca, C. S., Sutton, M., He, Y., ... Cooke, D. G. (2019). Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite. Science Advances, 5(5), [eaaw5558]. https://doi.org/10.1126/sciadv.aaw5558

Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite. / Lan, Yang; Dringoli, Benjamin J.; Valverde-Chávez, David A.; Ponseca, Carlito S.; Sutton, Mark; He, Yihui; Kanatzidis, Mercouri G; Cooke, David G.

In: Science Advances, Vol. 5, No. 5, eaaw5558, 31.05.2019.

Research output: Contribution to journalArticle

Lan, Y, Dringoli, BJ, Valverde-Chávez, DA, Ponseca, CS, Sutton, M, He, Y, Kanatzidis, MG & Cooke, DG 2019, 'Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite', Science Advances, vol. 5, no. 5, eaaw5558. https://doi.org/10.1126/sciadv.aaw5558
Lan Y, Dringoli BJ, Valverde-Chávez DA, Ponseca CS, Sutton M, He Y et al. Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite. Science Advances. 2019 May 31;5(5). eaaw5558. https://doi.org/10.1126/sciadv.aaw5558
Lan, Yang ; Dringoli, Benjamin J. ; Valverde-Chávez, David A. ; Ponseca, Carlito S. ; Sutton, Mark ; He, Yihui ; Kanatzidis, Mercouri G ; Cooke, David G. / Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite. In: Science Advances. 2019 ; Vol. 5, No. 5.
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