Intrinsic femtosecond charge generation dynamics in single crystal CH3NH3PbI3

David A. Valverde-Chávez, Carlito S. Ponseca, Constantinos C. Stoumpos, Arkady Yartsev, Mercouri G Kanatzidis, Villy Sundström, David G. Cooke

Research output: Contribution to journalArticle

99 Citations (Scopus)

Abstract

Hybrid metal-organic perovskite solar cells have astounded the solar cell community with their rapid rise in efficiency while maintaining low-cost fabrication. The intrinsic material photophysics related to the generation of free charges, their dynamics and efficiency, however, remains to be understood. As fabrication techniques improve, larger crystal grain sizes have been shown to be a critical factor for improving both the optical and transport properties of the hybrid metal halide perovskites. In this work, we use pulses of multi-THz frequency light in the ultra-broadband 1-30 THz (4-125 meV) range to observe the ac conductivity in large single crystal CH3NH3PbI3. Our spectra reveal the ultrafast dynamics and efficiencies of free charge creation and extremely high charge carrier mobility as high as 500-800 cm2 V-1 s-1. While quasi-equilibrium analysis of efficiencies through the Saha equation suggests a binding energy on the order of 49 meV, an observed reflectance feature appearing at high pump fluence occurs at 12 meV and is consistent with an orbital transition of the exciton, indicating a much lower Rydberg energy of 17 meV at room temperature. The signature of the exciton is found to vanish on a 1 ps time scale commensurate with the appearance of mobile carriers, consistent with thermal dissociation of the exciton to the continuum in the room temperature tetragonal phase.

Original languageEnglish
Pages (from-to)3700-3707
Number of pages8
JournalEnergy and Environmental Science
Volume8
Issue number12
DOIs
Publication statusPublished - Dec 1 2015

Fingerprint

Single crystals
Excitons
crystal
halide
metal
perovskite
energy
reflectance
pump
conductivity
grain size
temperature
Metal halides
timescale
Fabrication
Carrier mobility
Electron transitions
Binding energy
Charge carriers
cost

ASJC Scopus subject areas

  • Renewable Energy, Sustainability and the Environment
  • Environmental Chemistry
  • Pollution
  • Nuclear Energy and Engineering

Cite this

Valverde-Chávez, D. A., Ponseca, C. S., Stoumpos, C. C., Yartsev, A., Kanatzidis, M. G., Sundström, V., & Cooke, D. G. (2015). Intrinsic femtosecond charge generation dynamics in single crystal CH3NH3PbI3 Energy and Environmental Science, 8(12), 3700-3707. https://doi.org/10.1039/c5ee02503f

Intrinsic femtosecond charge generation dynamics in single crystal CH3NH3PbI3 . / Valverde-Chávez, David A.; Ponseca, Carlito S.; Stoumpos, Constantinos C.; Yartsev, Arkady; Kanatzidis, Mercouri G; Sundström, Villy; Cooke, David G.

In: Energy and Environmental Science, Vol. 8, No. 12, 01.12.2015, p. 3700-3707.

Research output: Contribution to journalArticle

Valverde-Chávez, DA, Ponseca, CS, Stoumpos, CC, Yartsev, A, Kanatzidis, MG, Sundström, V & Cooke, DG 2015, 'Intrinsic femtosecond charge generation dynamics in single crystal CH3NH3PbI3 ', Energy and Environmental Science, vol. 8, no. 12, pp. 3700-3707. https://doi.org/10.1039/c5ee02503f
Valverde-Chávez DA, Ponseca CS, Stoumpos CC, Yartsev A, Kanatzidis MG, Sundström V et al. Intrinsic femtosecond charge generation dynamics in single crystal CH3NH3PbI3 Energy and Environmental Science. 2015 Dec 1;8(12):3700-3707. https://doi.org/10.1039/c5ee02503f
Valverde-Chávez, David A. ; Ponseca, Carlito S. ; Stoumpos, Constantinos C. ; Yartsev, Arkady ; Kanatzidis, Mercouri G ; Sundström, Villy ; Cooke, David G. / Intrinsic femtosecond charge generation dynamics in single crystal CH3NH3PbI3 In: Energy and Environmental Science. 2015 ; Vol. 8, No. 12. pp. 3700-3707.
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