Spatially heterogeneous chlorine incorporation in organic-inorganic perovskite solar cells

Yanqi Luo; Shany Gamliel; Sally Nijem; Sigalit Aharon; Martin Holt; Benjamin Stripe; Volker Rose; Mariana I. Bertoni; Lioz Etgar; David P. Fenning

doi:10.1021/acs.chemmater.6b02065

Spatially heterogeneous chlorine incorporation in organic-inorganic perovskite solar cells

Yanqi Luo, Shany Gamliel, Sally Nijem, Sigalit Aharon, Martin Holt, Benjamin Stripe, Volker Rose, Mariana I. Bertoni, Lioz Etgar, David P. Fenning^*

^*Corresponding author for this work

Institute of Chemistry

Research output: Contribution to journal › Article › peer-review

36 Scopus citations

Abstract

Spatial heterogeneities in the chemical makeup of thin film photovoltaic devices are pivotal in determining device efficiency. We report the in-plane spatial distribution and degree of chlorine incorporation in organic-inorganic lead halide perovskite absorbers by means of nondestructive synchrotron-based nanoprobe X-ray fluorescence. The presence of chlorine is positively identified in CH₃NH₃PbI₃ films synthesized with Cl-containing precursors and as an impurity in some films synthesized with nominally Cl-free precursors. The impurity may be introduced from precursors or as contaminants during film synthesis. The films formed from Cl-containing precursors contain roughly an order of magnitude higher amount of chlorine, with Cl:I values greater than 0.02 found whether Cl is present in either the organic or the inorganic precursor for both one- and two-step fabrication processes. A spatial variation in the Cl incorporation is observed within single particles and as well as between particles within a given film, and the standard deviation of the Cl:I ratio across the films is up to 30% of the average value. Understanding and controlling the heterogeneous distribution of chlorine in hybrid perovskite layers may offer a path to improve their photovoltaic performance.

Original language	American English
Pages (from-to)	6536-6543
Number of pages	8
Journal	Chemistry of Materials
Volume	28
Issue number	18
DOIs	https://doi.org/10.1021/acs.chemmater.6b02065
State	Published - 27 Sep 2016

Bibliographical note

Funding Information:
The authors gratefully acknowledge Peter Fueszs experimental assistance at the beamline, and Yang Shao-Horn's helpful support and discussions. Y.L. acknowledges the support of the UC Carbon Neutrality Initiative and DPF start-up funds from the University of California, San Diego. L.E. acknowledges the Tashtiot Project of the Ofice of the Chief Scientist, and the German Israel Foundation for Young Researchers. This research used resources of both the Center for Nanoscale materials and the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

Publisher Copyright:
© 2016 American Chemical Society.

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10.1021/acs.chemmater.6b02065

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title = "Spatially heterogeneous chlorine incorporation in organic-inorganic perovskite solar cells",

abstract = "Spatial heterogeneities in the chemical makeup of thin film photovoltaic devices are pivotal in determining device efficiency. We report the in-plane spatial distribution and degree of chlorine incorporation in organic-inorganic lead halide perovskite absorbers by means of nondestructive synchrotron-based nanoprobe X-ray fluorescence. The presence of chlorine is positively identified in CH3NH3PbI3 films synthesized with Cl-containing precursors and as an impurity in some films synthesized with nominally Cl-free precursors. The impurity may be introduced from precursors or as contaminants during film synthesis. The films formed from Cl-containing precursors contain roughly an order of magnitude higher amount of chlorine, with Cl:I values greater than 0.02 found whether Cl is present in either the organic or the inorganic precursor for both one- and two-step fabrication processes. A spatial variation in the Cl incorporation is observed within single particles and as well as between particles within a given film, and the standard deviation of the Cl:I ratio across the films is up to 30% of the average value. Understanding and controlling the heterogeneous distribution of chlorine in hybrid perovskite layers may offer a path to improve their photovoltaic performance.",

author = "Yanqi Luo and Shany Gamliel and Sally Nijem and Sigalit Aharon and Martin Holt and Benjamin Stripe and Volker Rose and Bertoni, {Mariana I.} and Lioz Etgar and Fenning, {David P.}",

note = "Funding Information: The authors gratefully acknowledge Peter Fueszs experimental assistance at the beamline, and Yang Shao-Horn's helpful support and discussions. Y.L. acknowledges the support of the UC Carbon Neutrality Initiative and DPF start-up funds from the University of California, San Diego. L.E. acknowledges the Tashtiot Project of the Ofice of the Chief Scientist, and the German Israel Foundation for Young Researchers. This research used resources of both the Center for Nanoscale materials and the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

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AU - Holt, Martin

AU - Stripe, Benjamin

AU - Rose, Volker

AU - Bertoni, Mariana I.

AU - Etgar, Lioz

AU - Fenning, David P.

N1 - Funding Information: The authors gratefully acknowledge Peter Fueszs experimental assistance at the beamline, and Yang Shao-Horn's helpful support and discussions. Y.L. acknowledges the support of the UC Carbon Neutrality Initiative and DPF start-up funds from the University of California, San Diego. L.E. acknowledges the Tashtiot Project of the Ofice of the Chief Scientist, and the German Israel Foundation for Young Researchers. This research used resources of both the Center for Nanoscale materials and the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2016 American Chemical Society.

PY - 2016/9/27

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N2 - Spatial heterogeneities in the chemical makeup of thin film photovoltaic devices are pivotal in determining device efficiency. We report the in-plane spatial distribution and degree of chlorine incorporation in organic-inorganic lead halide perovskite absorbers by means of nondestructive synchrotron-based nanoprobe X-ray fluorescence. The presence of chlorine is positively identified in CH3NH3PbI3 films synthesized with Cl-containing precursors and as an impurity in some films synthesized with nominally Cl-free precursors. The impurity may be introduced from precursors or as contaminants during film synthesis. The films formed from Cl-containing precursors contain roughly an order of magnitude higher amount of chlorine, with Cl:I values greater than 0.02 found whether Cl is present in either the organic or the inorganic precursor for both one- and two-step fabrication processes. A spatial variation in the Cl incorporation is observed within single particles and as well as between particles within a given film, and the standard deviation of the Cl:I ratio across the films is up to 30% of the average value. Understanding and controlling the heterogeneous distribution of chlorine in hybrid perovskite layers may offer a path to improve their photovoltaic performance.

AB - Spatial heterogeneities in the chemical makeup of thin film photovoltaic devices are pivotal in determining device efficiency. We report the in-plane spatial distribution and degree of chlorine incorporation in organic-inorganic lead halide perovskite absorbers by means of nondestructive synchrotron-based nanoprobe X-ray fluorescence. The presence of chlorine is positively identified in CH3NH3PbI3 films synthesized with Cl-containing precursors and as an impurity in some films synthesized with nominally Cl-free precursors. The impurity may be introduced from precursors or as contaminants during film synthesis. The films formed from Cl-containing precursors contain roughly an order of magnitude higher amount of chlorine, with Cl:I values greater than 0.02 found whether Cl is present in either the organic or the inorganic precursor for both one- and two-step fabrication processes. A spatial variation in the Cl incorporation is observed within single particles and as well as between particles within a given film, and the standard deviation of the Cl:I ratio across the films is up to 30% of the average value. Understanding and controlling the heterogeneous distribution of chlorine in hybrid perovskite layers may offer a path to improve their photovoltaic performance.

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JO - Chemistry of Materials

JF - Chemistry of Materials

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ER -

Spatially heterogeneous chlorine incorporation in organic-inorganic perovskite solar cells

Abstract

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