The Origin of Open-Circuit Voltage Losses in Perovskite Solar Cells Investigated by Surface Photovoltage Measurement

Increasing the open circuit voltage (Voc) is one of the key strategies for further improvement of the efficiency of perovskite solar cells. It requires fundamental understanding of the complex optoelectronic processes related to charge carrier generation, transport, extraction and their loss mechanisms inside a device upon illumination. Herein we report the important origin of Voc losses in methylammonium lead iodide perovskite (MAPI) based solar cells, which results from undesirable positive charge (hole) accumulation at the interface between the perovskite photoactive layer and the PEDOT:PSS hole transport layer. We show strong correlation between the thickness-dependent surface photovoltage and device performance, unraveling that the interfacial charge accumulation leads to charge carrier recombination and results in a large decrease in Voc for the PEDOT:PSS/MAPI inverted devices (180 mV reduction in 50-nm-thick device compared to 230-nm-thick one). In contrast, accumulated positive charges at the TiO2...