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

Liam Collins; Eric S Muckley; Hsinhan Tsai; Dibyajyoti Ghosh; Amanda J Neukirch; Sergei Tretiak; Sergei V Kalinin; Wanyi Nie; Ilia N Ivanov

doi:10.1021/acsami.0c00561

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

ACS Appl Mater Interfaces. 2020 Apr 1;12(13):15380-15388. doi: 10.1021/acsami.0c00561. Epub 2020 Mar 20.

Authors

Liam Collins¹, Eric S Muckley¹, Hsinhan Tsai², Dibyajyoti Ghosh², Amanda J Neukirch², Sergei Tretiak², Sergei V Kalinin¹, Wanyi Nie², Ilia N Ivanov¹

Affiliations

¹ Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.
² Materials Physics and Application Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States.

PMID: 32159935
DOI: 10.1021/acsami.0c00561

Abstract

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-xFA_xCs_0.05PbI₃). We show that A-site cation composition defines charge transport mechanisms across broad temporal (10²-10^-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.

Keywords: hybrid organic−inorganic perovskites (HOIP); impedance spectroscopy (IS); ion transport; macroscale; nanoscale; time-resolved Kelvin probe force microscopy (tr-KPFM).