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Title: Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties

Abstract

In this paper, the nanoscale through-film and lateral photo-response and conductivity of large-grained methylammonium lead iodide (MAPbI 3) thin films are studied. In perovskite solar cells (PSC), these films result in efficiencies >17%. The grain boundaries (GBs) show high resistance at the top surface of the film, and act as an impediment to photocurrent collection. However, lower resistance pathways between grains exist below the top surface of the film, indicating that there exists a depth-dependent resistance of GBs (R GB(z)). Furthermore, lateral conductivity measurements indicate that R GB(z) exhibits GB-to-GB heterogeneity. These results indicate that increased photocurrent collection along GBs is not a prerequisite for high-efficiency PSCs. Rather, better control of depth-dependent GB electrical properties, and an improvement in the homogeneity of the GB-to-GB electrical properties, must be managed to enable further improvements in PSC efficiency. Finally, these results refute the implicit assumption seen in the literature that the electrical properties of GBs, as measured at the top surface of the perovskite film, necessarily reflect the electrical properties of GBs within the thickness of the film.

Authors:
 [1];  [2];  [3];  [1];  [3];  [4];  [2];  [1]
  1. National Inst. of Standards and Technology (NIST), Boulder, CO (United States). Material Measurement Lab., Applied Chemicals and Materials Division
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center
  3. National Inst. of Standards and Technology (NIST), Boulder, CO (United States). Physical Measurement Lab., Applied Physics Division
  4. National Renewable Energy Lab. (NREL), Golden, CO (United States). National Center for Photovoltaics
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1339245
Report Number(s):
NREL/JA-5900-67690
Journal ID: ISSN 1754-5692; EESNBY
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 9; Journal Issue: 12; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; nanoscale; methylammonium lead iodide thin films

Citation Formats

MacDonald, Gordon A., Yang, Mengjin, Berweger, Samuel, Killgore, Jason P., Kabos, Pavel, Berry, Joseph J., Zhu, Kai, and DelRio, Frank W. Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties. United States: N. p., 2016. Web. doi:10.1039/C6EE01889K.
MacDonald, Gordon A., Yang, Mengjin, Berweger, Samuel, Killgore, Jason P., Kabos, Pavel, Berry, Joseph J., Zhu, Kai, & DelRio, Frank W. Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties. United States. https://doi.org/10.1039/C6EE01889K
MacDonald, Gordon A., Yang, Mengjin, Berweger, Samuel, Killgore, Jason P., Kabos, Pavel, Berry, Joseph J., Zhu, Kai, and DelRio, Frank W. Fri . "Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties". United States. https://doi.org/10.1039/C6EE01889K. https://www.osti.gov/servlets/purl/1339245.
@article{osti_1339245,
title = {Methylammonium lead iodide grain boundaries exhibit depth-dependent electrical properties},
author = {MacDonald, Gordon A. and Yang, Mengjin and Berweger, Samuel and Killgore, Jason P. and Kabos, Pavel and Berry, Joseph J. and Zhu, Kai and DelRio, Frank W.},
abstractNote = {In this paper, the nanoscale through-film and lateral photo-response and conductivity of large-grained methylammonium lead iodide (MAPbI3) thin films are studied. In perovskite solar cells (PSC), these films result in efficiencies >17%. The grain boundaries (GBs) show high resistance at the top surface of the film, and act as an impediment to photocurrent collection. However, lower resistance pathways between grains exist below the top surface of the film, indicating that there exists a depth-dependent resistance of GBs (RGB(z)). Furthermore, lateral conductivity measurements indicate that RGB(z) exhibits GB-to-GB heterogeneity. These results indicate that increased photocurrent collection along GBs is not a prerequisite for high-efficiency PSCs. Rather, better control of depth-dependent GB electrical properties, and an improvement in the homogeneity of the GB-to-GB electrical properties, must be managed to enable further improvements in PSC efficiency. Finally, these results refute the implicit assumption seen in the literature that the electrical properties of GBs, as measured at the top surface of the perovskite film, necessarily reflect the electrical properties of GBs within the thickness of the film.},
doi = {10.1039/C6EE01889K},
url = {https://www.osti.gov/biblio/1339245}, journal = {Energy & Environmental Science},
issn = {1754-5692},
number = 12,
volume = 9,
place = {United States},
year = {2016},
month = {9}
}

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Works referenced in this record:

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Benefit of Grain Boundaries in Organic–Inorganic Halide Planar Perovskite Solar Cells
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journal, October 2014


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Transformation of the Excited State and Photovoltaic Efficiency of CH 3 NH 3 PbI 3 Perovskite upon Controlled Exposure to Humidified Air
journal, January 2015

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Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9%
journal, August 2012


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    Oriented Grains with Preferred Low-Angle Grain Boundaries in Halide Perovskite Films by Pressure-Induced Crystallization
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    Perovskite Solar Cells: From the Atomic Level to Film Quality and Device Performance
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    Capturing the Sun: A Review of the Challenges and Perspectives of Perovskite Solar Cells
    journal, January 2018


    Impact of Structural Dynamics on the Optical Properties of Methylammonium Lead Iodide Perovskites
    journal, June 2017


    Perowskit-Solarzellen: atomare Ebene, Schichtqualität und Leistungsfähigkeit der Zellen
    journal, February 2018


    Tin( iv ) dopant removal through anti-solvent engineering enabling tin based perovskite solar cells with high charge carrier mobilities
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    Identifying the charge generation dynamics in Cs + -based triple cation mixed perovskite solar cells
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    Imaging material functionality through three-dimensional nanoscale tracking of energy flow
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    Edge Effect on the Population of Free Carriers and Excitons in Single‐Crystal CH 3 NH 3 PbBr 3 Perovskite Nanomaterials
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    Defect Engineering toward Highly Efficient and Stable Perovskite Solar Cells
    journal, July 2018


    Approaching the Shockley–Queisser limit for fill factors in lead–tin mixed perovskite photovoltaics
    journal, January 2020


    Imaging Metal Halide Perovskites Material and Properties at the Nanoscale
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    Interface Engineering in Tin Perovskite Solar Cells
    journal, October 2019