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In this study we analysed halide perovskite films deposited directly on crystalline silicon by means of two set-ups using different operating modes of the surface photovoltage (SPV) methods, i.e., the Kelvin probe force microscopy (KPFM) and the metal-insulator-semiconductor (MIS) technique. The KPFM allowed to visualize surface potential distribution on a microscale while MIS technique allowed to study SPV spectral dependence. We studied wavelength dependent SPV of these samples, which allowed us to effectively vary the probe depth in the sample and discern the contribution from each interface to the overall effect measured under white light illumination. Depending on where the photocarriers are generated, different SPV signals are observed: at the perovskite/Si interface, the signal depends on Si doping type, while at the surface the SPV is always negative indicating downward surface band bending. This is confirmed by analysing SPV phase measured in the AC MIS mode. In addition, distinction between slow and fast processes contributing to measured SPV was possible. It has been observed, that with decreasing the illumination wavelength, the processes causing SPV become slower, which can indicate that high energy photons not only generate electronic photocarriers but can also induce chemical changes with creation of defects or ionic species that also modify the measured SPV.

Lead halide perovskites are semiconductor materials which are employed as nonintentionally doped absorbers inserted between two selective carrier transport layers (SCTL), realizing a p‐i‐n or n‐i‐p heterojunction. In our study, we have developed and investigated a lateral device, based on methylammonium lead iodide (MAPbI3) in which the p‐i‐n heterojunction develops in the horizontal direction. Our research suggests that the effective doping level in the MAPbI3 film should be very low, below 1012 cm−3. Along the vertical direction, this doping level is not enough to screen the electric field of the buried heterojunction with the SCTL. The perovskite work function is therefore affected by the work function of the SCTL underneath. From drift‐diffusion simulations, we show that intrinsic perovskite‐SCTL structures develop mV range surface photovoltages (SPVs) under continuous illumination. However, perovskite‐SCTL structures can develop SPVs of hundreds of mV, as confirmed by our measurements. We therefore analyzed the compatibility between low doping and low defect densities in the perovskite layer and such high SPV values using numerical modeling. It is shown that these high SPV values could originate from electronic processes due to large band offsets in the buried perovskite‐SCTL heterojunctions, or at the SCTL‐transparent conductive oxide (TCO) buried heterojunction. However, such electronic processes can hardly explain the long SPV persistence after switching off the illumination. [ABSTRACT FROM AUTHOR]