Phase Segregation Mechanisms in Mixed-Halide CsPb(BrxI1-x)3 Nanocrystals in Dependence of Their Sizes and Their Initial [Br]:[I] Ratios

Hannah Funk; Tal Binyamin; Lioz Etgar; Oleksandra Shargaieva; Thomas Unold; Alberto Eljarrat; Christoph T. Koch; Daniel Abou-Ras

doi:10.1021/acsmaterialsau.3c00056

Phase Segregation Mechanisms in Mixed-Halide CsPb(Br_xI_1-x)₃ Nanocrystals in Dependence of Their Sizes and Their Initial [Br]:[I] Ratios

Hannah Funk, Tal Binyamin, Lioz Etgar, Oleksandra Shargaieva, Thomas Unold, Alberto Eljarrat, Christoph T. Koch, Daniel Abou-Ras^*

^*Corresponding author for this work

Institute of Chemistry

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

2 Scopus citations

Abstract

Phase segregation in inorganic CsPb(Br_xI_1-x)₃ nanoparticles (NPs) exhibiting originally a homogeneous [Br]:[I] mixture was investigated by means of in situ transmission electron microscopy (TEM) and evaluated by using multivariate analyses. The colloidal synthesis of the NPs offers good control of the halide ratios on the nanoscale. The spatially resolved TEM investigations were correlated with integral photoluminescence measurements. By this approach, the halide-segregation processes and their spatial distributions can be described as being governed by the interaction of three partial processes: electron- and photon-irradiation-induced iodide oxidation, local differences in band gap energy, and intrinsic lattice strain. Since the oxidation can be induced by both electron-beam and light irradiation, both irradiation types can induce phase segregation in CsPb(Br_xI_1-x)₃ compounds. This makes in situ TEM a valuable tool to monitor phase transformation in corresponding NPs and thin films on the sub-nm scale.

Original language	English
Pages (from-to)	687-698
Number of pages	12
Journal	ACS Materials Au
Volume	3
Issue number	6
DOIs	https://doi.org/10.1021/acsmaterialsau.3c00056
State	Published - 8 Nov 2023

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

Keywords

in situ monitoring
mixed-halide perovskite nanocrystals
multivariate analysis
phase segregation
transmission electron microscopy

Access to Document

10.1021/acsmaterialsau.3c00056

Cite this

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title = "Phase Segregation Mechanisms in Mixed-Halide CsPb(BrxI1-x)3 Nanocrystals in Dependence of Their Sizes and Their Initial [Br]:[I] Ratios",

abstract = "Phase segregation in inorganic CsPb(BrxI1-x)3 nanoparticles (NPs) exhibiting originally a homogeneous [Br]:[I] mixture was investigated by means of in situ transmission electron microscopy (TEM) and evaluated by using multivariate analyses. The colloidal synthesis of the NPs offers good control of the halide ratios on the nanoscale. The spatially resolved TEM investigations were correlated with integral photoluminescence measurements. By this approach, the halide-segregation processes and their spatial distributions can be described as being governed by the interaction of three partial processes: electron- and photon-irradiation-induced iodide oxidation, local differences in band gap energy, and intrinsic lattice strain. Since the oxidation can be induced by both electron-beam and light irradiation, both irradiation types can induce phase segregation in CsPb(BrxI1-x)3 compounds. This makes in situ TEM a valuable tool to monitor phase transformation in corresponding NPs and thin films on the sub-nm scale.",

keywords = "in situ monitoring, mixed-halide perovskite nanocrystals, multivariate analysis, phase segregation, transmission electron microscopy",

author = "Hannah Funk and Tal Binyamin and Lioz Etgar and Oleksandra Shargaieva and Thomas Unold and Alberto Eljarrat and Koch, {Christoph T.} and Daniel Abou-Ras",

note = "Publisher Copyright: {\textcopyright} 2023 The Authors. Published by American Chemical Society.",

year = "2023",

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AU - Etgar, Lioz

AU - Shargaieva, Oleksandra

AU - Unold, Thomas

AU - Eljarrat, Alberto

AU - Koch, Christoph T.

AU - Abou-Ras, Daniel

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N2 - Phase segregation in inorganic CsPb(BrxI1-x)3 nanoparticles (NPs) exhibiting originally a homogeneous [Br]:[I] mixture was investigated by means of in situ transmission electron microscopy (TEM) and evaluated by using multivariate analyses. The colloidal synthesis of the NPs offers good control of the halide ratios on the nanoscale. The spatially resolved TEM investigations were correlated with integral photoluminescence measurements. By this approach, the halide-segregation processes and their spatial distributions can be described as being governed by the interaction of three partial processes: electron- and photon-irradiation-induced iodide oxidation, local differences in band gap energy, and intrinsic lattice strain. Since the oxidation can be induced by both electron-beam and light irradiation, both irradiation types can induce phase segregation in CsPb(BrxI1-x)3 compounds. This makes in situ TEM a valuable tool to monitor phase transformation in corresponding NPs and thin films on the sub-nm scale.

AB - Phase segregation in inorganic CsPb(BrxI1-x)3 nanoparticles (NPs) exhibiting originally a homogeneous [Br]:[I] mixture was investigated by means of in situ transmission electron microscopy (TEM) and evaluated by using multivariate analyses. The colloidal synthesis of the NPs offers good control of the halide ratios on the nanoscale. The spatially resolved TEM investigations were correlated with integral photoluminescence measurements. By this approach, the halide-segregation processes and their spatial distributions can be described as being governed by the interaction of three partial processes: electron- and photon-irradiation-induced iodide oxidation, local differences in band gap energy, and intrinsic lattice strain. Since the oxidation can be induced by both electron-beam and light irradiation, both irradiation types can induce phase segregation in CsPb(BrxI1-x)3 compounds. This makes in situ TEM a valuable tool to monitor phase transformation in corresponding NPs and thin films on the sub-nm scale.

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