Validated Analysis of Component Distribution Inside Perovskite Solar Cells and Its Utility in Unveiling Factors of Device Performance and Degradation.

Time-of-flight secondary-ion mass spectrometry (ToF-SIMS) has been used for gaining insights into perovskite solar cells (PSCs). However, the importance of selecting ion beam parameters to eliminate artifacts in the resulting depth profile is often overlooked. In this work, significant artifacts were identified with commonly applied sputter sources, i.e., an O beam and an Ar-gas cluster ion beam (Ar-GCIB), which could lead to misinterpretation of the PSC structure. On the other hand, polyatomic C and Ar ion beams were found to be able to produce depth profiles that properly reflect the distribution of the components. On the basis of this validated method, differences in component distribution, depending on the fabrication processes, were identified and discussed. The solvent-engineering process yielded a homogeneous film with higher device performance, but sequential deposition led to a perovskite layer sandwiched by methylammonium-deficient layers that impeded the performance. For device degradation, it was found that most components remained intact at their original position except for iodide. This result unambiguously indicated that iodide diffusion was one of the key factors governing the device lifetime. With the validated parameters provided, ToF-SIMS was demonstrated as a powerful tool to unveil the structure variation amid device performance and during degradation, which are crucial for the future development of PSCs.