NiO_x Passivation in Perovskite Solar Cells: From Surface Reactivity to Device Performance

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Abstract

Nonstoichiometric nickel oxide (NiO_x) is one of the very few metal oxides successfully used as hole extraction layer in p-i-n type perovskite solar cells (PSCs). Its favorable optoelectronic properties and facile large-scale preparation methods are potentially relevant for future commercialization of PSCs, though currently low operational stability of PSCs is reported when a NiO_x hole extraction layer is used in direct contact with the perovskite absorber. Poorly understood degradation reactions at this interface are seen as cause for the inferior stability, and a variety of interface passivation approaches have been shown to be effective in improving the overall solar cell performance. To gain a better understanding of the processes happening at this interface, we systematically passivated specific defects on NiO_x with three different categories of organic/inorganic compounds. The effects on NiO_x and the perovskite (MAPbI₃) deposited on top were investigated using X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and scanning electron microscopy (SEM). Here, we find that the perovskite's structural stability and film formation can be significantly affected by the passivation treatment of the NiO_x surface. In combination with density functional theory (DFT) calculations, a likely origin of NiO_x-perovskite degradation interactions is proposed. The surface passivated NiO_x layers were incorporated into MAPbI₃-based PSCs, and the influence on device performance and operational stability was investigated by current-voltage (J-V) characterization, impedance spectroscopy (IS), and open circuit voltage decay (OCVD) measurements. Interestingly, we find that a superior structural stability due to interface passivation must not relate to high operational stability. The discrepancy comes from the formation of excess ions at the interface, which negatively impacts all solar cell parameters.

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