Publication date: 1st July 2014
Organometal halide perovskites have recently attracted enormous attention since MeNH3PbX3 can be successfully applied as photoactive material in photovoltaic devices, yielding solar cells with an efficiency exceeding 15%. Surprisingly, the exact mechanism how charges are generated and transported so well is unclear. In this work, we investigated the charge carrier generation, mobility and recombination in MeNH3PbI3. For MeNH3PbI3 deposited on Al2O3 we observed fast formation of microsecond lived charge carriers on pulsed laser excitation in the visible at 300 K using time resolved photoconductivity measurements with terahertz radiation or microwaves as probe. At low laser fluences a maximum charge carrier mobility of about 5 cm2/Vs, yielding charge carrier diffusion lengths well above 5 μm are found. At higher laser intensities higher order recombination processes become operative lowering the mobile charge carrier population rapidly with a rate constant of, γ= 13×10-10 cm3s-1. Reducing the temperature results in increasing charge carrier mobilities following a T-1.6 dependence, which we attribute to a reduction in phonon scattering (Σµ = 16 cm2/Vs at 165K). Despite the fact that Sµ increases on lowering the temperature, γ diminishes with a factor six implying that charge recombination in MeNH3PbI3 is temperature activated. For MeNH3PbI3 deposited on charge carrier specific electrodes, such as TiO2 and PCBM lower signal sizes are found which are explained by the rapid collection of one type of carrier by the electrode. Those collected carriers have lower mobilities leading to a reduction of signal size and, in addition to different decay kinetics. The results underline the importance of the perovskite crystal structure, the exciton binding energy and the activation energy for recombination as key factors in optimizing new perovskite materials.