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 (ε_r) 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 ε_r 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 ε_r 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.