Time-Resolved Changes in Dielectric Constant of Metal Halide Perovskites under Illumination

Despite their impressive performance as a solar absorber, much remains unknown on the fundamental properties of metal halide perovskites (MHPs). Their polar nature in particular is an intense area of study, and the relative permittivity (εr) is a parameter widely used to quantify polarization over a range of different time scales. In this report, we have exploited frequency-dependent time-resolved microwave conductivity (TRMC) to study how εr values of a range of MHPs change as a function of time, upon optical illumination. Further characterization of charge carriers and polarizability are conducted by femtosecond transient absorption and stimulated Raman spectroscopy. We find that changes in εr are roughly proportional to photogenerated carrier density but decay with a shorter time constant than conductance, suggesting that the presence of charge carriers alone does not determine polarization.