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Title: Hyperspectral mapping of nanoscale photophysics and degradation processes in hybrid perovskite at the single grain level

Abstract

With solar cells reaching 26.1% certified efficiency, hybrid perovskites are now the most efficient thin film photovoltaic material. Though substantial effort has focussed on synthesis approaches and device architectures to further improve perovskite-based solar cells, more work is needed to correlate physical properties of the underlying film structure with device performance. Here, using cathodoluminescence microscopy coupled with unsupervised machine learning, we quantify how nanoscale heterogeneity globally builds up within a large morphological grain of hybrid perovskite when exposed to extrinsic stimuli such as charge accumulation from electron beams or milder environmental factors like humidity. The converged electron-beam excitation allows us to map PbI2 and the emergence of other intermediate phases with high spatial and energy resolution. In contrast with recent reports of hybrid perovskite cathodoluminescence, we observe no significant change in the PbI2 signatures, even after high-energy electron beam excitation. In fact, we can exploit the stable PbI2 signatures to quantitatively map how hybrid perovskites degrade. Moreover, we show how our methodology allows disentangling of the photophysics associated with photon recycling and band-edge emission with sub-micron resolution using a fundamental understanding of electron interactions in hybrid perovskites.

Authors:
 [1];  [2];  [1];  [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Department of Physics, University of Alabama at Birmingham, 1300 University Blvd., Birmingham AL, 35294 USA
  2. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
  3. Clarion University, 840 Wood St, Clarion, PA 16214, USA
  4. Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA, Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Aeronautics and Space Administration (NASA)
OSTI Identifier:
1996604
Alternate Identifier(s):
OSTI ID: 2000413
Grant/Contract Number:  
AC05-00OR22725; 80NSSC19M0051
Resource Type:
Published Article
Journal Name:
Nanoscale Advances
Additional Journal Information:
Journal Name: Nanoscale Advances Journal Volume: 5 Journal Issue: 18; Journal ID: ISSN 2516-0230
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Taylor, Ethan J., Iyer, Vasudevan, Dhami, Bibek S., Klein, Clay, Lawrie, Benjamin J., and Appavoo, Kannatassen. Hyperspectral mapping of nanoscale photophysics and degradation processes in hybrid perovskite at the single grain level. United Kingdom: N. p., 2023. Web. doi:10.1039/D3NA00529A.
Taylor, Ethan J., Iyer, Vasudevan, Dhami, Bibek S., Klein, Clay, Lawrie, Benjamin J., & Appavoo, Kannatassen. Hyperspectral mapping of nanoscale photophysics and degradation processes in hybrid perovskite at the single grain level. United Kingdom. https://doi.org/10.1039/D3NA00529A
Taylor, Ethan J., Iyer, Vasudevan, Dhami, Bibek S., Klein, Clay, Lawrie, Benjamin J., and Appavoo, Kannatassen. Tue . "Hyperspectral mapping of nanoscale photophysics and degradation processes in hybrid perovskite at the single grain level". United Kingdom. https://doi.org/10.1039/D3NA00529A.
@article{osti_1996604,
title = {Hyperspectral mapping of nanoscale photophysics and degradation processes in hybrid perovskite at the single grain level},
author = {Taylor, Ethan J. and Iyer, Vasudevan and Dhami, Bibek S. and Klein, Clay and Lawrie, Benjamin J. and Appavoo, Kannatassen},
abstractNote = {With solar cells reaching 26.1% certified efficiency, hybrid perovskites are now the most efficient thin film photovoltaic material. Though substantial effort has focussed on synthesis approaches and device architectures to further improve perovskite-based solar cells, more work is needed to correlate physical properties of the underlying film structure with device performance. Here, using cathodoluminescence microscopy coupled with unsupervised machine learning, we quantify how nanoscale heterogeneity globally builds up within a large morphological grain of hybrid perovskite when exposed to extrinsic stimuli such as charge accumulation from electron beams or milder environmental factors like humidity. The converged electron-beam excitation allows us to map PbI2 and the emergence of other intermediate phases with high spatial and energy resolution. In contrast with recent reports of hybrid perovskite cathodoluminescence, we observe no significant change in the PbI2 signatures, even after high-energy electron beam excitation. In fact, we can exploit the stable PbI2 signatures to quantitatively map how hybrid perovskites degrade. Moreover, we show how our methodology allows disentangling of the photophysics associated with photon recycling and band-edge emission with sub-micron resolution using a fundamental understanding of electron interactions in hybrid perovskites.},
doi = {10.1039/D3NA00529A},
journal = {Nanoscale Advances},
number = 18,
volume = 5,
place = {United Kingdom},
year = {Tue Sep 12 00:00:00 EDT 2023},
month = {Tue Sep 12 00:00:00 EDT 2023}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/D3NA00529A

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