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Title: Oxygen-induced defects at the lead halide perovskite/graphene oxide interfaces

Abstract

Here, graphene oxide or its reduced derivative (GO/RGO) replace metal oxides in perovskite photovoltaics to achieve energy band alignment for minimization of the energy barriers at the film interfaces allowing efficient charge transport, and eliminate stability issues. However, the power conversion efficiencies fall in a wide range (~0.6–18%). Therefore, the perovskite growth and nucleation on GO/RGO require fundamental understanding to improve device function for controlled fabrication, which remain a major challenge. We analyze the surface morphology and crystallization of the lead halide perovskites (MAPbX3) at 20–300 °C on GO using X-ray diffraction and photoelectron spectroscopy. To determine defect mechanisms and their composition, we perform in situ transmission infrared and micro Raman spectroscopy, and the cross-sectional scanning microscopy that captures interfacial imperfections with the oxygen defects. We demonstrate the oxygen-induced defects at the MAPbX3/GO interfaces that initiate at room temperature, and occur through the nucleophilic substitution reactions. Unexpectedly, structural defects nucleate in GO forming chemically reduced GO, and modify the surface morphology that yield a poor perovskite growth. Our theoretical studies also reveal that energetically favorable, exothermic reactions between the halides of the perovskite precursors and the oxygen groups of GO generate acidic reaction by-products (i.e. HX), that confirm the formationmore » of oxygen-induced defects.« less

Authors:
ORCiD logo [1];  [2];  [1];  [2];  [1]
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  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Ulsan National Institute of Science and Technology, Ulsan (Korea)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1422395
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 4; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Acik, Muge, Park, In Kee, Koritala, Rachel E., Lee, Geunsik, and Rosenberg, Richard A. Oxygen-induced defects at the lead halide perovskite/graphene oxide interfaces. United States: N. p., 2017. Web. doi:10.1039/c7ta10010h.
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Acik, Muge, Park, In Kee, Koritala, Rachel E., Lee, Geunsik, & Rosenberg, Richard A. Oxygen-induced defects at the lead halide perovskite/graphene oxide interfaces. United States. https://doi.org/10.1039/c7ta10010h
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Acik, Muge, Park, In Kee, Koritala, Rachel E., Lee, Geunsik, and Rosenberg, Richard A. Thu . "Oxygen-induced defects at the lead halide perovskite/graphene oxide interfaces". United States. https://doi.org/10.1039/c7ta10010h. https://www.osti.gov/servlets/purl/1422395.
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@article{osti_1422395,
title = {Oxygen-induced defects at the lead halide perovskite/graphene oxide interfaces},
author = {Acik, Muge and Park, In Kee and Koritala, Rachel E. and Lee, Geunsik and Rosenberg, Richard A.},
abstractNote = {Here, graphene oxide or its reduced derivative (GO/RGO) replace metal oxides in perovskite photovoltaics to achieve energy band alignment for minimization of the energy barriers at the film interfaces allowing efficient charge transport, and eliminate stability issues. However, the power conversion efficiencies fall in a wide range (~0.6–18%). Therefore, the perovskite growth and nucleation on GO/RGO require fundamental understanding to improve device function for controlled fabrication, which remain a major challenge. We analyze the surface morphology and crystallization of the lead halide perovskites (MAPbX3) at 20–300 °C on GO using X-ray diffraction and photoelectron spectroscopy. To determine defect mechanisms and their composition, we perform in situ transmission infrared and micro Raman spectroscopy, and the cross-sectional scanning microscopy that captures interfacial imperfections with the oxygen defects. We demonstrate the oxygen-induced defects at the MAPbX3/GO interfaces that initiate at room temperature, and occur through the nucleophilic substitution reactions. Unexpectedly, structural defects nucleate in GO forming chemically reduced GO, and modify the surface morphology that yield a poor perovskite growth. Our theoretical studies also reveal that energetically favorable, exothermic reactions between the halides of the perovskite precursors and the oxygen groups of GO generate acidic reaction by-products (i.e. HX), that confirm the formation of oxygen-induced defects.},
doi = {10.1039/c7ta10010h},
journal = {Journal of Materials Chemistry. A},
number = 4,
volume = 6,
place = {United States},
year = {Thu Dec 21 00:00:00 EST 2017},
month = {Thu Dec 21 00:00:00 EST 2017}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1039/c7ta10010h
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Figures / Tables:

Figure 1 Figure 1: Photos of a) as-prepared GO (3-5 layers) deposited on a quartz piece, b) after spin coating (40 μl solution, at a spin rate of 4000 rpm, 30s) of methylammonium bromide and lead bromide at 40 wt.% in DMF at room temperature, and c) after annealing at 130°C formore » 1 hr to grow MAPbBr3. SEM images of d) MAPbBr3, after spin coating of the precursors on a Si/SiO2 substrate at 130°C. SEM images of spin-coated precursors of e) MABr and PbBr on a GO (3-5 layers) thin film at room temperature, and f) after annealing at 130°C for MAPbBr3 on GO. The scale bars for each SEM image indicates 1 μm.« less
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