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Transformation from crystalline precursor to perovskite in PbCl2-derived MAPbI3

Stone, Kevin H. ; Gold-Parker, Aryeh ; Pool, Vanessa L. ; Unger, Eva L. LU ; Bowring, Andrea R. ; McGehee, Michael D. ; Toney, Michael F. and Tassone, Christopher J. (2018) In Nature Communications 9(1).
Abstract

Understanding the formation chemistry of metal halide perovskites is key to optimizing processing conditions and realizing enhanced optoelectronic properties. Here, we reveal the structure of the crystalline precursor in the formation of methylammonium lead iodide (MAPbI3) from the single-step deposition of lead chloride and three equivalents of methylammonium iodide (PbCl2 + 3MAI) (MA = CH3NH3). The as-spun film consists of crystalline MA2PbI3Cl, which is composed of one-dimensional chains of lead halide octahedra, coexisting with disordered MACl. We show that the transformation of precursor into perovskite is not favored in the presence of MACl, and thus the gradual... (More)

Understanding the formation chemistry of metal halide perovskites is key to optimizing processing conditions and realizing enhanced optoelectronic properties. Here, we reveal the structure of the crystalline precursor in the formation of methylammonium lead iodide (MAPbI3) from the single-step deposition of lead chloride and three equivalents of methylammonium iodide (PbCl2 + 3MAI) (MA = CH3NH3). The as-spun film consists of crystalline MA2PbI3Cl, which is composed of one-dimensional chains of lead halide octahedra, coexisting with disordered MACl. We show that the transformation of precursor into perovskite is not favored in the presence of MACl, and thus the gradual evaporation of MACl acts as a self-regulating mechanism to slow the conversion. We propose the stable precursor phase enables dense film coverage and the slow transformation may lead to improved crystal quality. This enhanced chemical understanding is paramount for the rational control of film deposition and the fabrication of superior optoelectronic devices.

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author
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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Nature Communications
volume
9
issue
1
article number
3458
publisher
Nature Publishing Group
external identifiers
  • pmid:30150720
  • scopus:85052289263
ISSN
2041-1723
DOI
10.1038/s41467-018-05937-4
language
English
LU publication?
yes
id
cfff7d6e-e1f6-488a-8606-360c993a4424
date added to LUP
2018-09-24 14:32:34
date last changed
2024-04-29 13:44:00
@article{cfff7d6e-e1f6-488a-8606-360c993a4424,
  abstract     = {{<p>Understanding the formation chemistry of metal halide perovskites is key to optimizing processing conditions and realizing enhanced optoelectronic properties. Here, we reveal the structure of the crystalline precursor in the formation of methylammonium lead iodide (MAPbI<sub>3</sub>) from the single-step deposition of lead chloride and three equivalents of methylammonium iodide (PbCl<sub>2</sub> + 3MAI) (MA = CH<sub>3</sub>NH<sub>3</sub>). The as-spun film consists of crystalline MA<sub>2</sub>PbI<sub>3</sub>Cl, which is composed of one-dimensional chains of lead halide octahedra, coexisting with disordered MACl. We show that the transformation of precursor into perovskite is not favored in the presence of MACl, and thus the gradual evaporation of MACl acts as a self-regulating mechanism to slow the conversion. We propose the stable precursor phase enables dense film coverage and the slow transformation may lead to improved crystal quality. This enhanced chemical understanding is paramount for the rational control of film deposition and the fabrication of superior optoelectronic devices.</p>}},
  author       = {{Stone, Kevin H. and Gold-Parker, Aryeh and Pool, Vanessa L. and Unger, Eva L. and Bowring, Andrea R. and McGehee, Michael D. and Toney, Michael F. and Tassone, Christopher J.}},
  issn         = {{2041-1723}},
  language     = {{eng}},
  month        = {{08}},
  number       = {{1}},
  publisher    = {{Nature Publishing Group}},
  series       = {{Nature Communications}},
  title        = {{Transformation from crystalline precursor to perovskite in PbCl<sub>2</sub>-derived MAPbI<sub>3</sub>}},
  url          = {{http://dx.doi.org/10.1038/s41467-018-05937-4}},
  doi          = {{10.1038/s41467-018-05937-4}},
  volume       = {{9}},
  year         = {{2018}},
}