Slow cooling of hot polarons in halide perovskite solar cells
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Accepted version
Published version
Author(s)
Frost, JM
Whalley, LD
Walsh, A
Type
Journal Article
Abstract
Halide perovskites show unusual thermalisation kinetics for above bandgap
photo-excitation. We explain this as a consequence of excess energy being
deposited into discrete large polaron states. The cross-over between
low-fluence and high-fluence `phonon bottleneck' cooling is due to a Mott
transition where the polarons overlap ($n \ge 10^{18}/\mathrm{cm}^3$) and the
phonon sub-populations are shared. We calculate the initial rate of cooling
(thermalisation) from the scattering time in the Fr\"ohlich polaron model to be
78 meVps$^{-1}$ for $\mathrm{CH}_3\mathrm{NH}_3\mathrm{PbI}_3$. This rapid
initial thermalisation 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 ultra-low thermal conductivity of the
perovskite lattice.
photo-excitation. We explain this as a consequence of excess energy being
deposited into discrete large polaron states. The cross-over between
low-fluence and high-fluence `phonon bottleneck' cooling is due to a Mott
transition where the polarons overlap ($n \ge 10^{18}/\mathrm{cm}^3$) and the
phonon sub-populations are shared. We calculate the initial rate of cooling
(thermalisation) from the scattering time in the Fr\"ohlich polaron model to be
78 meVps$^{-1}$ for $\mathrm{CH}_3\mathrm{NH}_3\mathrm{PbI}_3$. This rapid
initial thermalisation 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 ultra-low thermal conductivity of the
perovskite lattice.
Date Issued
2017-10-23
Date Acceptance
2017-10-23
Citation
ACS Energy Letters, 2017, 2, pp.2647-2652
ISSN
2380-8195
Publisher
American Chemical Society
Start Page
2647
End Page
2652
Journal / Book Title
ACS Energy Letters
Volume
2
Copyright Statement
This is an open access article published under a Creative Commons Attribution (CC-BY)
License, which permits unrestricted use, distribution and reproduction in any medium,
provided the author and source are cited.
License, which permits unrestricted use, distribution and reproduction in any medium,
provided the author and source are cited.
License URL
Subjects
cond-mat.mtrl-sci
cond-mat.mtrl-sci
Notes
7 pages, 1 schematic, 3 figures
Publication Status
Published
Date Publish Online
2017-10-23