Charge-Carrier Dynamics in Hybrid Metal Halide Perovskites
Laura Herz a
a Department of Physics, University of Oxford, Clarendon Laboratory, Parks Road, Oxford OX1 3PU, United Kingdom
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe September Meeting 2015 (NFM15)
Santiago de Compostela, Spain, 2015 September 6th - 15th
Invited Speaker, Laura Herz, presentation 303
Publication date: 8th June 2015

We have elucidated the charge-carrier dynamics in organic-inorganic metal halide perovskites that are implemented as active light-harvesting materials in high-efficiency solar cells. We found that charge carriers can travel over distances of up to a micron in solution-processed CH3NH3PbI3−xClx perovskite absorbers [1], thus making these materials suitable for planar-heterojunction solar cells. We demonstrate [2,3] that this effect arises from a combination of high charge-carrier mobility (11.6 cm2 V−1 s−1 for mesostructured solution-processed, and 33 cm2 V−1 s−1 for evaporated CH3NH3PbI3−xClx films) and abnormally low bi-molecular charge recombination rates that defy the Langevin limit by at least four orders of magnitude. We further show that CH3NH3PbI3−xCl films exhibit extraordinarily low energetic disorder, with an emission spectrum that is predominantly homogenously broadened through strong coupling of charge-carriers to phonons [4]. With the observed spectral width of 103 meV, such gain media can sustain amplification of light pulses as short as 6.4 fs, opening a perspective for electrically-pumped femtosecond-pulsed lasers.In addition, we have examined the charge-carrier dynamics in the lead-free perovskite CH3NH3SnI3 for which solar cells processed on a mesoporous TiO2 scaffold were shown to reach efficiencies of over 6% [5]. Using transient THz spectroscopy, we find that the ultrafast charge-dynamics are dominated by a first-order decay that may originate from electron recombination with an unintentional hole doping density of ~1018 cm-3. We establish an effective charge-carrier mobility of 1.6 cm2 V−1 s−1, yielding a charge-carrier diffusion length of 30nm [5]. We show that if mono-molecular processes arising from unintentional doping or charge trapping are resolved, charge diffusion lengths in excess of one micron can be reached for CH3NH3SnI3, opening the way for lead-free perovskite photovoltaics with planar-heterojunction architecture.



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