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Unravelling the mechanism of photoinduced charge transfer processes in lead iodide perovskite solar cells


Lead halide perovskites have recently been used as light absorbers in hybrid organic–inorganic solid-state solar cells, with efficiencies as high as 15% and open-circuit voltages of 1 V. However, a detailed explanation of the mechanisms of operation within this photovoltaic system is still lacking. Here, we investigate the photoinduced charge transfer processes at the surface of the perovskite using time-resolved techniques. Transient laser spectroscopy and microwave photoconductivity measurements were applied to TiO2 and Al2O3 mesoporous films impregnated with CH3NH3PbI3 perovskite and the organic hole-transporting material spiro-OMeTAD. We show that primary charge separation occurs at both junctions, with TiO2 and the hole-transporting material, simultaneously, with ultrafast electron and hole injection taking place from the photoexcited perovskite over similar timescales. Charge recombination is shown to be significantly slower on TiO2 than on Al2O3 films.

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Figure 1
Figure 2: Time evolution of electron and hole populations in photoexcited CH3NH3PbI3 perovskite in various systems.
Figure 3: Transient microwave photoconductance measurements of the perovskite material deposited on various substrates.
Figure 4: Charge recombination dynamics obtained from nanosecond-laser flash photolysis of the various systems.


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Financial support was provided by the Swiss National Science Foundation and the NCCR-MUST programme. M.G. and J.T. acknowledge the European Research Council (ERC) for an Advanced Research Grant (ARG no. 247404) funded under the ‘Mesolight’ project. A.M. and J.-E.M. thank J. Burschka, A. Dualeh, S. M. Zakeeruddin and C. Grätzel for discussions, P. Comte for the preparation of Al2O3 paste, P. Gao for the preparation of CH3NH3I, A. Devižis for help with near-infrared detection and A. Gasperini for atomic force microscopy measurements.

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A.M. designed the experiments and prepared the samples. A.M. and J.T. carried out the laser experiments and analysed the data with J.-E.M. T.M. and D.F. designed the photoconductance experiments. D.F. performed the microwave experiments on the samples prepared by T.M. and analysed the data with the help of T.M., M.K. and R.vdK. A.M. prepared the manuscript with the help of J.T. and J.-E.M. J.-E.M. designed the femtosecond and nanosecond experimental spectroscopy tools, conceived the project and directed the work. All other authors discussed the results and commented on the manuscript.

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Correspondence to Jacques-E. Moser.

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The authors declare no competing financial interests.

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Marchioro, A., Teuscher, J., Friedrich, D. et al. Unravelling the mechanism of photoinduced charge transfer processes in lead iodide perovskite solar cells. Nature Photon 8, 250–255 (2014).

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