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Title: Halide Heterogeneity Affects Local Charge Carrier Dynamics in Mixed-Ion Lead Perovskite Thin Films

Abstract

The mechanisms and elemental composition that form the basis for the improved optical and electronic properties in mixed-ion perovskite solar cells are still not well understood compared to standard methylammonium lead triiodide perovskite devices. Here, we use synchrotron-based X-ray fluorescence to map the composition of perovskite thin films. To get insights into the elemental distribution during film growth, we fabricate films with three different thicknesses. To create a link between the composition and the electronic properties, we perform Kelvin probe force microscopy and time-resolved photoluminescence spectroscopy. We find that the elemental composition is highly dependent on the film thickness, in particular, that the I/Pb ratio is altered for single grains based on the film thickness. The difference in the I/Pb ratio reveals to be the root cause for the underlying difference in film lifetime and defect density influencing charge carrier dynamics. Our results provide an in-depth analysis approach combining macro- and nanoscale techniques to shed light onto the fundamental processes which help to further engineer perovskite thin films and improve device efficiencies.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [3];  [3];  [3];  [3];  [4];  [4];  [3];  [5];  [5]; ORCiD logo [4];  [3]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Florida State Univ., Tallahassee, FL (United States)
  2. Harvard Univ., Cambridge, MA (United States)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  4. Florida State Univ., Tallahassee, FL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1557609
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 31; Journal Issue: 10; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wieghold, Sarah, Tresback, Jason, Correa-Baena, Juan-Pablo, Hartono, Noor Titan Putri, Sun, Shijing, Liu, Zhe, Layurova, Mariya, VanOrman, Zachary A., Bieber, Alexander S., Thapa, Janak, Lai, Barry, Cai, Zhonghou, Nienhaus, Lea, and Buonassisi, Tonio. Halide Heterogeneity Affects Local Charge Carrier Dynamics in Mixed-Ion Lead Perovskite Thin Films. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b00650.
Wieghold, Sarah, Tresback, Jason, Correa-Baena, Juan-Pablo, Hartono, Noor Titan Putri, Sun, Shijing, Liu, Zhe, Layurova, Mariya, VanOrman, Zachary A., Bieber, Alexander S., Thapa, Janak, Lai, Barry, Cai, Zhonghou, Nienhaus, Lea, & Buonassisi, Tonio. Halide Heterogeneity Affects Local Charge Carrier Dynamics in Mixed-Ion Lead Perovskite Thin Films. United States. https://doi.org/10.1021/acs.chemmater.9b00650
Wieghold, Sarah, Tresback, Jason, Correa-Baena, Juan-Pablo, Hartono, Noor Titan Putri, Sun, Shijing, Liu, Zhe, Layurova, Mariya, VanOrman, Zachary A., Bieber, Alexander S., Thapa, Janak, Lai, Barry, Cai, Zhonghou, Nienhaus, Lea, and Buonassisi, Tonio. Mon . "Halide Heterogeneity Affects Local Charge Carrier Dynamics in Mixed-Ion Lead Perovskite Thin Films". United States. https://doi.org/10.1021/acs.chemmater.9b00650. https://www.osti.gov/servlets/purl/1557609.
@article{osti_1557609,
title = {Halide Heterogeneity Affects Local Charge Carrier Dynamics in Mixed-Ion Lead Perovskite Thin Films},
author = {Wieghold, Sarah and Tresback, Jason and Correa-Baena, Juan-Pablo and Hartono, Noor Titan Putri and Sun, Shijing and Liu, Zhe and Layurova, Mariya and VanOrman, Zachary A. and Bieber, Alexander S. and Thapa, Janak and Lai, Barry and Cai, Zhonghou and Nienhaus, Lea and Buonassisi, Tonio},
abstractNote = {The mechanisms and elemental composition that form the basis for the improved optical and electronic properties in mixed-ion perovskite solar cells are still not well understood compared to standard methylammonium lead triiodide perovskite devices. Here, we use synchrotron-based X-ray fluorescence to map the composition of perovskite thin films. To get insights into the elemental distribution during film growth, we fabricate films with three different thicknesses. To create a link between the composition and the electronic properties, we perform Kelvin probe force microscopy and time-resolved photoluminescence spectroscopy. We find that the elemental composition is highly dependent on the film thickness, in particular, that the I/Pb ratio is altered for single grains based on the film thickness. The difference in the I/Pb ratio reveals to be the root cause for the underlying difference in film lifetime and defect density influencing charge carrier dynamics. Our results provide an in-depth analysis approach combining macro- and nanoscale techniques to shed light onto the fundamental processes which help to further engineer perovskite thin films and improve device efficiencies.},
doi = {10.1021/acs.chemmater.9b00650},
journal = {Chemistry of Materials},
number = 10,
volume = 31,
place = {United States},
year = {Mon Apr 29 00:00:00 EDT 2019},
month = {Mon Apr 29 00:00:00 EDT 2019}
}

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