Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic–Inorganic Perovskites on Macro- and Nanoscales

Progress in flexible organic electronics necessitates a full understanding of how local inhomogeneities impact electronic and ionic conduction pathways and underlie macroscopic device characteristics. We used frequency- and time-resolved macro- and nanoprobe measurements to study spatiotemporal characteristics of multiscale charge transport dynamics in a series of ternary-blended hybrid organic inorganic perovskites (HOIPs) (MA 0.95- x FA x Cs 0.05 PbI 3 ). We show that A-site cation composition defines charge transport mechanisms across broad temporal (10 2 -10 -6 s) and spatial (millimeters-picometers) scales. Ab initio molecular dynamic simulations suggest that insertion of FA results in a dynamic lattice, improved ion transport, and dipole screening. We demonstrate that correlations between macro- and nanoscale measurements provide a pathway for accessing distribution of relaxation in nanoscale polarization and charge transport dynamics of ionically conductive functional perovskites.