Abstract
Understanding the nature of photogenerated carriers and their subsequent dynamics in perovskites is important for the development of related materials and devices. Most ultrafast dynamic measurements on the perovskite materials were conducted under high carrier densities, which likely obscures the genuine dynamics at low carrier densities under solar illumination conditions. In this study, we presented a detailed experimental study of the carrier density-dependent dynamics in hybrid lead iodide perovskites using a highly sensitive transient absorption spectrometer. We found that the carrier lifetime was about a hundred nanosecond in the linear response range, representing sunlight excitation, which was much longer than under high carrier densities. We also elucidated that the fast carrier decay (<1 ps) and the medium decay processes (tens of ps) occurred via the defect state trapping, and we determined its effects on the utilization percentage of photogenerated carriers through quantitative analysis. Furthermore, we obtained the Shockley-Queisser limit that took into account the carrier trapping effect, which directly reflected the material performance.