Abstract
Abstract Nickel oxide (NiOx) has exhibited great potential as an inorganic hole transport layer (HTL) in perovskite solar cells (PSCs) due to its wide optical bandgap and superior stability. In this study, we have modulated the Ni2+ vacancies in NiOx film by controlling deposition temperature in a hot-casting process, resulting the change of coordination structure and charge state of NiOx. Moreover, the change of the HOMO level of NiOx makes it more compatible with perovskite to decrease energy losses and enhance hole carrier injection efficiency. Besides, the defect modulation in the electronic structure of NiOx is beneficial for increasing the electrical conductivity and mobility, which are considered to achieve the balance of charge carrier transport and avoid charge accumulation at the interface between perovskite and HTL effectively. Both experimental analyses and theoretical calculations reveal the increase of nickel vacancy defects change the electronic structure of NiOx by increasing the ratio of Ni3+/Ni2+ and improving the p-type characteristics. Accordingly, an optimal deposition temperature at 120 °C enabled a 36.24% improvement in the power conversion efficiency compared to that deposited at room temperature (25 °C). Therefore, this work provides a facile method to manipulate the electronic structure of NiOx to improve the charge carrier transport and photovoltaic performance of related PSCs.
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