Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells

Jarvist Moore Frost, Lucy D. Whalley, Aron Walsh

Research output: Contribution to journalArticle

36 Citations (Scopus)

Abstract

Halide perovskites show unusual thermalization kinetics for above-bandgap photoexcitation. We explain this as a consequence of excess energy being deposited into discrete large polaron states. The crossover between low-fluence and high-fluence "phonon bottleneck" cooling is due to a Mott transition where the polarons overlap (n ≥ 1018 cm-3) and the phonon subpopulations are shared. We calculate the initial rate of cooling (thermalization) from the scattering time in the Fröhlich polaron model to be 78 meV ps-1 for CH3NH3PbI3. This rapid initial thermalization involves heat transfer into optical phonon modes coupled by a polar dielectric interaction. Further cooling to equilibrium over hundreds of picoseconds is limited by the ultralow thermal conductivity of the perovskite lattice.

Original languageEnglish
Pages (from-to)2647-2652
Number of pages6
JournalACS Energy Letters
Volume2
Issue number12
DOIs
Publication statusPublished - 2017 Dec 8

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Polarons
Gene Conversion
Cooling
Photoexcitation
Electron transitions
Perovskite
Thermal conductivity
Energy gap
Scattering
Heat transfer
Kinetics
Perovskite solar cells

All Science Journal Classification (ASJC) codes

  • Chemistry (miscellaneous)
  • Renewable Energy, Sustainability and the Environment
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Materials Chemistry

Cite this

Frost, Jarvist Moore ; Whalley, Lucy D. ; Walsh, Aron. / Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells. In: ACS Energy Letters. 2017 ; Vol. 2, No. 12. pp. 2647-2652.
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Slow Cooling of Hot Polarons in Halide Perovskite Solar Cells. / Frost, Jarvist Moore; Whalley, Lucy D.; Walsh, Aron.

In: ACS Energy Letters, Vol. 2, No. 12, 08.12.2017, p. 2647-2652.

Research output: Contribution to journalArticle

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