Correlation of annealing time with crystal structure, composition, and electronic properties of CH3NH3PbI3-xClx mixed-halide perovskite films

Maryline Ralaiarisoa, Yan Busby, Jean-Jacques Pireaux, Johannes Frisch, Ingo Salzmann, Norbert Koch

Research output: Contribution to journalArticle

Abstract

Using 3D imaging with time-of-flight secondary ion mass spectrometry (ToF-SIMS) complemented by grazing-incidence X-ray diffraction (GIXRD), we spatially resolve changes in both the composition and structure of CH3NH3I3-xClx perovskite films on conducting polymer substrates at different annealing stages, in particular, before and after complete perovskite crystallization. The early stage of annealing is characterized by phase separation throughout the entire film into domains with perovskite and domains with a dominating chloride-rich phase. After sufficiently long annealing, one single perovskite phase of homogeneous composition on the (lateral) micrometer scale is observed, along with pronounced film texture. This composition evolution is accompanied by diffusion of chloride from the perovskite layer towards the conducting polymer substrate, and even accumulation there. Photoelectron spectroscopy analysis further shows that perovskite films become increasingly n-type with annealing time and upon full conversion, which correlates with the change of film composition. Our results accentuate the importance of chloride for the formation of crystalline and textured films, which are crucial for enhancing the PV performance of perovskite-based solar cells.

Original languageEnglish
Pages (from-to)828-836
Number of pages9
JournalPhysical Chemistry Chemical Physics
Volume19
Issue number1
DOIs
Publication statusPublished - 21 Dec 2016

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Electronic properties
Perovskite
halides
Crystal structure
Annealing
crystal structure
annealing
Chemical analysis
electronics
chlorides
Chlorides
conducting polymers
Conducting polymers
grazing incidence
secondary ion mass spectrometry
Substrates
Photoelectron spectroscopy
Secondary ion mass spectrometry
Crystallization
perovskite

Cite this

@article{4072be57948b4f2f8a37e2d7826c921e,
title = "Correlation of annealing time with crystal structure, composition, and electronic properties of CH3NH3PbI3-xClx mixed-halide perovskite films",
abstract = "Using 3D imaging with time-of-flight secondary ion mass spectrometry (ToF-SIMS) complemented by grazing-incidence X-ray diffraction (GIXRD), we spatially resolve changes in both the composition and structure of CH3NH3I3-xClx perovskite films on conducting polymer substrates at different annealing stages, in particular, before and after complete perovskite crystallization. The early stage of annealing is characterized by phase separation throughout the entire film into domains with perovskite and domains with a dominating chloride-rich phase. After sufficiently long annealing, one single perovskite phase of homogeneous composition on the (lateral) micrometer scale is observed, along with pronounced film texture. This composition evolution is accompanied by diffusion of chloride from the perovskite layer towards the conducting polymer substrate, and even accumulation there. Photoelectron spectroscopy analysis further shows that perovskite films become increasingly n-type with annealing time and upon full conversion, which correlates with the change of film composition. Our results accentuate the importance of chloride for the formation of crystalline and textured films, which are crucial for enhancing the PV performance of perovskite-based solar cells.",
author = "Maryline Ralaiarisoa and Yan Busby and Jean-Jacques Pireaux and Johannes Frisch and Ingo Salzmann and Norbert Koch",
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publisher = "Royal Society of Chemistry",
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Correlation of annealing time with crystal structure, composition, and electronic properties of CH3NH3PbI3-xClx mixed-halide perovskite films. / Ralaiarisoa, Maryline; Busby, Yan; Pireaux, Jean-Jacques; Frisch, Johannes; Salzmann, Ingo; Koch, Norbert.

In: Physical Chemistry Chemical Physics, Vol. 19, No. 1, 21.12.2016, p. 828-836.

Research output: Contribution to journalArticle

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T1 - Correlation of annealing time with crystal structure, composition, and electronic properties of CH3NH3PbI3-xClx mixed-halide perovskite films

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AU - Frisch, Johannes

AU - Salzmann, Ingo

AU - Koch, Norbert

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AB - Using 3D imaging with time-of-flight secondary ion mass spectrometry (ToF-SIMS) complemented by grazing-incidence X-ray diffraction (GIXRD), we spatially resolve changes in both the composition and structure of CH3NH3I3-xClx perovskite films on conducting polymer substrates at different annealing stages, in particular, before and after complete perovskite crystallization. The early stage of annealing is characterized by phase separation throughout the entire film into domains with perovskite and domains with a dominating chloride-rich phase. After sufficiently long annealing, one single perovskite phase of homogeneous composition on the (lateral) micrometer scale is observed, along with pronounced film texture. This composition evolution is accompanied by diffusion of chloride from the perovskite layer towards the conducting polymer substrate, and even accumulation there. Photoelectron spectroscopy analysis further shows that perovskite films become increasingly n-type with annealing time and upon full conversion, which correlates with the change of film composition. Our results accentuate the importance of chloride for the formation of crystalline and textured films, which are crucial for enhancing the PV performance of perovskite-based solar cells.

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