Effects of interfacial energy level alignment on carrier dynamics and photovoltaic performance of inverted perovskite solar cells

Abstract Metal doping is an efficient method for optimizing NiOx as hole transport material in the inverted perovskite solar cells, which can contribute to the optimization of the interfacial energy level alignment, while the underlying influencing mechanism on the charge carrier dynamics and device performance needs to be further elucidated. In this work, NiOx films with modulated energy levels are obtained via Li doping and examined by ultraviolet photoelectron spectrometer. The effects of the energy level alignment of NiOx on the carrier transfer and recombination dynamics are elucidated by transient photovoltage/photocurrent and transient fluorescence dynamics. The Li doping can significantly shift the valence band of NiOx downward, and the 4% Li content endows NiOx with the optimal energy level matching with perovskite and the best charge separation/transfer ability, which can be confirmed through the photoluminescence results. The corresponding device possesses superior photovoltaic parameters with the champion power conversion efficiency of 17.34%, 37% higher than device based on pure NiOx. The results highlight that proper metal doping can optimize the energy level of the hole transport material to well match the perovskite, thus efficiently promoting charge separation and inhibiting charge recombination, which leads to the enhancement of the device performances.