Abstract

Impedance spectroscopy offers access to all the different electronic and ionic processes taking place simultaneously in an operating solar cell. To date, its use on perovskite solar cells has been challenging because of the richness of the physical processes occurring within similar time domains. The aim of this work is to understand the general impedance response and propose a general equivalent circuit model that accounts for the different processes and gives access to quantitative analysis. When the electron-selective contacts and the thickness of the perovskite film are systematically modified, it is possible to distinguish between the characteristic impedance signals of the perovskite layer and those arising from the contacts. The study is carried out using mixed organic lead halogen perovskite (FA(0.85)MA(0.15)Pb(I0.85Br0.15)(3)) solar cells with three different electron-selective contacts: SnO2, TiO2, and Nb2O5. The contacts have been deposited by atomic layer deposition (ALD), which provides pinhole-free films and excellent thickness control in the absence of a mesoporous layer to simplify the impedance analysis. It was found that the interfacial impedance has a rich structure that reveals different capacitive processes, serial steps for electron extraction, and a prominent inductive loop related to negative capacitance at intermediate frequencies. Overall, the present report provides insights into the impedance response of perovskite solar cells which enable an understanding of the different electronic and ionic processes taking place during device operation.

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