Monitoring Charge Separation of Individual Cells in Perovskite/Silicon Tandems via Transient Surface Photovoltage Spectroscopy

Identification of charge carrier separation processes in perovskite/silicon tandem solar cells and recombination at buried interfaces of charge selective contacts are crucial for photovoltaic research. Here, intensity- and wavelength-dependent transient surface photovoltage (tr-SPV) is used to investigate slot-die-coated perovskite top layers deposited on n-type heterojunction silicon bottom cells. We show that using an appropriate combination of photon energy and/or bottom cell polarity, one can individually probe the buried interfaces of the bottom silicon cell or the perovskite's buried interfaces of a tandem solar cell: for excitation with higher energy photons, time delays before the onset of a strong SPV signal indicate significant hole minority drift before separation in the silicon bottom cells. Furthermore, symmetric bottom Si heterojunction solar cell stacks can serve to investigate the top perovskite stack including its junction to the bottom cell, unhampered by photovoltages from the silicon substrate. Thus, investigation of the buried interfaces in tandem devices using time-resolved surface photovoltage is found to yield valuable information on charge carrier extraction at buried interfaces and demonstrates its unique potential compared to more conventional approaches that rely on photoluminescence decay kinetics.