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Title: Direct Correlation of Charge Carrier Transport to Local Crystal Quality in Lead Halide Perovskites

Abstract

Although solution processing methods provide an attractive route toward development of low-cost functional materials, these accessible fabrication approaches can engender high concentrations of microscopic structural defects that are detrimental to performance. In lead halide perovskites, structural disorder derived from solution processing has been implicated as an important determiner of photophysical properties. However, a direct correlation between the functional properties of these materials and the local crystal structure in which non-equilibrium states evolve has remained elusive, in part because structural heterogeneities occur on length scales that defy conventional characterization techniques. To address this knowledge gap, in this work we have combined ultrafast pump–probe microscopy and electron backscattering diffraction to directly correlate charge carrier transport with the local diffraction pattern contrast, an indicator of crystal quality. Spatial correlation of these measurements strongly suggests that even on individual single crystal CsPbBr3 domains, microscopic variability in the crystal quality profoundly impacts the efficiency of charge carrier transport.

Authors:
 [1]; ORCiD logo [1]
  1. Montana State Univ., Bozeman, MT (United States)
Publication Date:
Research Org.:
Montana State Univ., Bozeman, MT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Beckman Young Investigator Program; National Science Foundation (NSF)
OSTI Identifier:
1658903
Grant/Contract Number:  
SC0014128; 1632134
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 20; Journal Issue: 7; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Lead Halide Perovskite; Carrier Transport; Time-resolved Microscopy; Electron Diffraction

Citation Formats

Hickey, Casey L., and Grumstrup, Erik M. Direct Correlation of Charge Carrier Transport to Local Crystal Quality in Lead Halide Perovskites. United States: N. p., 2020. Web. doi:10.1021/acs.nanolett.0c01244.
Hickey, Casey L., & Grumstrup, Erik M. Direct Correlation of Charge Carrier Transport to Local Crystal Quality in Lead Halide Perovskites. United States. https://doi.org/10.1021/acs.nanolett.0c01244
Hickey, Casey L., and Grumstrup, Erik M. Wed . "Direct Correlation of Charge Carrier Transport to Local Crystal Quality in Lead Halide Perovskites". United States. https://doi.org/10.1021/acs.nanolett.0c01244. https://www.osti.gov/servlets/purl/1658903.
@article{osti_1658903,
title = {Direct Correlation of Charge Carrier Transport to Local Crystal Quality in Lead Halide Perovskites},
author = {Hickey, Casey L. and Grumstrup, Erik M.},
abstractNote = {Although solution processing methods provide an attractive route toward development of low-cost functional materials, these accessible fabrication approaches can engender high concentrations of microscopic structural defects that are detrimental to performance. In lead halide perovskites, structural disorder derived from solution processing has been implicated as an important determiner of photophysical properties. However, a direct correlation between the functional properties of these materials and the local crystal structure in which non-equilibrium states evolve has remained elusive, in part because structural heterogeneities occur on length scales that defy conventional characterization techniques. To address this knowledge gap, in this work we have combined ultrafast pump–probe microscopy and electron backscattering diffraction to directly correlate charge carrier transport with the local diffraction pattern contrast, an indicator of crystal quality. Spatial correlation of these measurements strongly suggests that even on individual single crystal CsPbBr3 domains, microscopic variability in the crystal quality profoundly impacts the efficiency of charge carrier transport.},
doi = {10.1021/acs.nanolett.0c01244},
journal = {Nano Letters},
number = 7,
volume = 20,
place = {United States},
year = {Wed Jun 10 00:00:00 EDT 2020},
month = {Wed Jun 10 00:00:00 EDT 2020}
}

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