Photoinduced Stark Effects and Mechanism of Ion Displacement in Perovskite Solar Cell Materials

Organometallic halide perovskites (OMHPs) have recently emerged as a promising class of materials in photovoltaic technology. Here, we present an in-depth investigation of the physics in these systems by measuring the photoinduced absorption (PIA) in OMHPs as a function of materials composition, excitation wavelength, and modulation frequency. We report a photoinduced Stark effect that depends on the excitation wavelength and on the dipole strength of the monovalent cations in the A position of the ABX₃ perovskite. The results presented are corroborated by density functional theory calculations and provide fundamental information about the photoinduced local electric field change under blue and red excitation as well as insights into the mechanism of light-induced ion displacement in OMHPs. For optimized perovskite solar cell devices beyond 19% efficiency, we show that excess thermalization energy of blue photons plays a role in overcoming the activation energy for ion diffusion.