Probing Perovskite Inhomogeneity beyond the Surface: TOF-SIMS Analysis of Halide Perovskite Photovoltaic Devices
Understanding the origins and evolution of inhomogeneity in halide perovskite solar cells appears to be a key to advancing the technology. Time-of-flight secondary-ion mass spectrometry (TOF-SIMS) is one of the few techniques that can obtain chemical information from all components of hybrid organic-inorganic perovskite photovoltaics in one dimension (standard depth profiling), two dimensions (high-resolution 100-nm imaging), as well as three dimensions (tomography combining high-resolution imaging with depth profiling). TOF-SIMS has been used to analyze perovskite photovoltaics made by a variety of methods, and the breadth of insight that can be gained from the technique is illustrated here including: cation uniformity (depth and lateral), changes in chemistry upon alternate processing, changes in chemistry upon degradation, and lateral distribution of additives that passivate grain boundaries. Using TOF-SIMS on multiple perovskite compositions, we show information regarding hybrid perovskite formation as well as inhomogeneity critical to device performance can be extracted providing one of the best proxies for understanding compositional changes resulting from degradation. Here, we also describe in detail the measurement artifacts and recommended best practices that enable unique insight regarding hybrid perovskite solar cell materials and devices.