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

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

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6 Scopus citations

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.

Original language	English
Pages (from-to)	15380-15388
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	12
Issue number	13
DOIs	https://doi.org/10.1021/acsami.0c00561
State	Published - Apr 1 2020

Funding

This research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. This work was supported in part by the Los Alamos National Laboratory (LANL) Directed Research and Development Funds (LDRD) and partly conducted at the Center for Nonlinear Studies and the Center for Integrated Nanotechnologies U.S. Department of Energy (DOE). This research used resources provided by the LANL Institutional Computing (IC) Program. LANL is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy (Contract 89233218NCA000001). This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. This work was supported in part by the Los Alamos National Laboratory (LANL) Directed Research and Development Funds (LDRD) and partly conducted at the Center for Nonlinear Studies and the Center for Integrated Nanotechnologies, U.S. Department of Energy (DOE). This research used resources provided by the LANL Institutional Computing (IC) Program. LANL is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy (Contract 89233218NCA000001). This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

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

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10.1021/acsami.0c00561

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Collins, L., Muckley, E. S., Tsai, H., Ghosh, D., Neukirch, A. J., Tretiak, S., Kalinin, S. V., Nie, W., & Ivanov, I. N. (2020). Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic-Inorganic Perovskites on Macro- And Nanoscales. ACS Applied Materials and Interfaces, 12(13), 15380-15388. https://doi.org/10.1021/acsami.0c00561

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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) (MA0.95-xFAxCs0.05PbI3). 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)",

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Collins, L, Muckley, ES, Tsai, H, Ghosh, D, Neukirch, AJ, Tretiak, S, Kalinin, SV, Nie, W & Ivanov, IN 2020, 'Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic-Inorganic Perovskites on Macro- And Nanoscales', ACS Applied Materials and Interfaces, vol. 12, no. 13, pp. 15380-15388. https://doi.org/10.1021/acsami.0c00561

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AU - Tsai, Hsinhan

AU - Ghosh, Dibyajyoti

AU - Neukirch, Amanda J.

AU - Tretiak, Sergei

AU - Kalinin, Sergei V.

AU - Nie, Wanyi

AU - Ivanov, Ilia N.

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AB - 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) (MA0.95-xFAxCs0.05PbI3). 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.

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

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