Exploring Responses of Contact Kelvin Probe Force Microscopy in Triple-Cation Double-Halide Perovskites
Abstract
Hybrid organic–inorganic perovskite (HOIP) solar cells have undergone unprecedentedly rapid improvement in power conversion efficiencies during the last decade, but controversy remains regarding the role of local phenomena and heterogeneity in grain by grain. These challenges in turn necessitate understanding the fundamental mechanisms operating at individual grains and exploring how these mechanisms give rise to the collective behaviors of the films. Although numerous efforts have targeted local phenomena in these materials using classical scanning probe microscopy modalities, the measurements remain difficult to interpret due to intrinsic coupling between possible ferroelectric, ion migration, bulk and surface electrochemical phenomena, and the effects of light on these behaviors. Here, we explore the electromechanical responses in (Cs0.05FA0.85MA0.15)Pb(I0.85Br0.15)3 perovskite thin film in the dark and under illumination using band excitation-piezoresponse force microscopy (BE-PFM). To identify and separate ferroic, electrostatic, and electrochemical responses, we utilize contact-Kelvin probe force microscopy (cKPFM). The cKPFM responses show weak variability with morphological features in the dark, while such variability significantly increases under illumination. Deconvolution of the cKPFM responses via principal component analysis (PCA) shows heterogeneity in grain to grain possibly due to variation in migration and segregation of halide ions in mixed perovskites at specific grains. Further, we propose anmore »
- Authors:
-
[1];
[2];
[1];
[3];
[2];
[2];
[1]
- Univ. of Tennessee, Knoxville, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- National Academy of Science of Ukraine, Kyiv (Ukraine)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1818661
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 125; Journal Issue: 22; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thin films; Grain; Electrostatics; Colloid; Polarization
Citation Formats
Kim, Dohyung, Vasudevan, Rama K., Higgins, Kate, Morozovska, Anna N., Eliseev, Eugene A., Ziatdinov, Maxim, Kalinin, Sergei V., and Ahmadi, Mahshid. Exploring Responses of Contact Kelvin Probe Force Microscopy in Triple-Cation Double-Halide Perovskites. United States: N. p., 2021.
Web. doi:10.1021/acs.jpcc.1c02474.
Kim, Dohyung, Vasudevan, Rama K., Higgins, Kate, Morozovska, Anna N., Eliseev, Eugene A., Ziatdinov, Maxim, Kalinin, Sergei V., & Ahmadi, Mahshid. Exploring Responses of Contact Kelvin Probe Force Microscopy in Triple-Cation Double-Halide Perovskites. United States. https://doi.org/10.1021/acs.jpcc.1c02474
Kim, Dohyung, Vasudevan, Rama K., Higgins, Kate, Morozovska, Anna N., Eliseev, Eugene A., Ziatdinov, Maxim, Kalinin, Sergei V., and Ahmadi, Mahshid. Fri .
"Exploring Responses of Contact Kelvin Probe Force Microscopy in Triple-Cation Double-Halide Perovskites". United States. https://doi.org/10.1021/acs.jpcc.1c02474. https://www.osti.gov/servlets/purl/1818661.
@article{osti_1818661,
title = {Exploring Responses of Contact Kelvin Probe Force Microscopy in Triple-Cation Double-Halide Perovskites},
author = {Kim, Dohyung and Vasudevan, Rama K. and Higgins, Kate and Morozovska, Anna N. and Eliseev, Eugene A. and Ziatdinov, Maxim and Kalinin, Sergei V. and Ahmadi, Mahshid},
abstractNote = {Hybrid organic–inorganic perovskite (HOIP) solar cells have undergone unprecedentedly rapid improvement in power conversion efficiencies during the last decade, but controversy remains regarding the role of local phenomena and heterogeneity in grain by grain. These challenges in turn necessitate understanding the fundamental mechanisms operating at individual grains and exploring how these mechanisms give rise to the collective behaviors of the films. Although numerous efforts have targeted local phenomena in these materials using classical scanning probe microscopy modalities, the measurements remain difficult to interpret due to intrinsic coupling between possible ferroelectric, ion migration, bulk and surface electrochemical phenomena, and the effects of light on these behaviors. Here, we explore the electromechanical responses in (Cs0.05FA0.85MA0.15)Pb(I0.85Br0.15)3 perovskite thin film in the dark and under illumination using band excitation-piezoresponse force microscopy (BE-PFM). To identify and separate ferroic, electrostatic, and electrochemical responses, we utilize contact-Kelvin probe force microscopy (cKPFM). The cKPFM responses show weak variability with morphological features in the dark, while such variability significantly increases under illumination. Deconvolution of the cKPFM responses via principal component analysis (PCA) shows heterogeneity in grain to grain possibly due to variation in migration and segregation of halide ions in mixed perovskites at specific grains. Further, we propose an electrostatic mechanism based on the physics of semiconductors, which can directly link the observed cKPFM behaviors with the ionic and electronic density of states (DOS) and their time dynamics. Here, these findings suggest that cKPFM is a powerful probe of local ionic behaviors on the nanoscale, both in HOIPs and other materials.},
doi = {10.1021/acs.jpcc.1c02474},
journal = {Journal of Physical Chemistry. C},
number = 22,
volume = 125,
place = {United States},
year = {Fri May 28 00:00:00 EDT 2021},
month = {Fri May 28 00:00:00 EDT 2021}
}
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