| Abstract: | Metal halide perovskite (MHP) solar cells have attracted much attention due to the rapidly growing power conversion efficiency that has reached 25.2% in a decade, comparable to established commercial photovoltaic modules. Compositional engineering is one of the most effective methods to boost the performance of MHP solar cells. Further improving the efficiency and the stability of MHP solar cells necessitates good understanding of the chemical–efficiency correlation and the chemical evolution during the degradation of MHP solar cells. In this regard, time‐of‐flight secondary ion mass spectrometry (ToF‐SIMS) is a powerful tool to investigate the chemical aspect of MHPs and has played an important role in advancing the development of MHP optoelectronics. However, up to date, a review that can guide future utilization of ToF‐SIMS in the MHP development is missing. Herein, the capabilities of ToF‐SIMS in MHP investigations are summarized and analyzed from simple material synthesis and chemical distribution to more complicated device operation mechanism and stability. The strength of ToF‐SIMS in resolving important issues in this field, such as interface composition, ion migration, and degradation in MHP is highlighted. Finally, an outlook with an emphasis on making the utmost of ToF‐SIMS in developing MHP devices is provided. |
