The Effects of Electronic Impurities and Electron–Hole Recombination Dynamics on Large-Grain Organic–Inorganic Perovskite Photovoltaic Efficiencies

Hybrid organic-inorganic perovskites have attracted considerable attention after promising developments in energy harvesting and other optoelectronic applications. However, further optimization will require a deeper understanding of the intrinsic photophysics of materials with relevant structural characteristics. Here, the dynamics of photoexcited charge carriers in large-area grain organic-inorganic perovskite thin films is investigated via confocal time-resolved photoluminescence spectroscopy. It is found that the bimolecular recombination of free charges is the dominant decay mechanism at excitation densities relevant for photovoltaic applications. Bimolecular coefficients are found to be on the order of 10⁻⁹ cm³ s⁻¹, comparable to typical direct-gap semiconductors, yet significantly smaller than theoretically expected. It is also demonstrated that there is no degradation in carrier transport in these thin films due to electronic impurities. Suppressed electron–hole recombination and transport that is not limited by deep level defects provide a microscopic model for the superior performance of large-area grain hybrid perovskites for photovoltaic applications.