4.8 Article

Observation of a hot-phonon bottleneck in lead-iodide perovskites

Journal

NATURE PHOTONICS
Volume 10, Issue 1, Pages 53-59

Publisher

NATURE PUBLISHING GROUP
DOI: 10.1038/NPHOTON.2015.213

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Funding

  1. Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy through the Solar Photochemistry programme [DE-AC36-08GO28308]
  2. US Department of Energy/National Renewable Energy Laboratory's Laboratory Directed Research and Development (LDRD) programme

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We study the carrier dynamics in planar methyl ammonium lead iodide perovskite films using broadband transient absorption spectroscopy. We show that the sharp optical absorption onset is due to an exciton transition that is inhomogeneously broadened with a binding energy of 9 meV. We fully characterize the transient absorption spectrum by free-carrier-induced bleaching of the exciton transition, quasi-Fermi energy, carrier temperature and bandgap renormalization constant. The photo-induced carrier temperature is extracted from the transient absorption spectra and monitored as a function of delay time for different excitation wavelengths and photon fluences. We find an efficient hot-phonon bottleneck that slows down cooling of hot carriers by three to four orders of magnitude in time above a critical injection carrier density of similar to 5x10(17) cm(-3). Compared with molecular beam epitaxially grown GaAs, the critical density is an order of magnitude lower and the relaxation time is approximately three orders of magnitude longer.

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