Proceedings of nanoGe September Meeting 2015 (NFM15)
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.