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Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals

[Image: see text] The vast majority of lead halide perovskite (LHP) nanocrystals (NCs) are currently based on either a single halide composition (CsPbCl(3), CsPbBr(3), and CsPbI(3)) or an alloyed mixture of bromide with either Cl(–) or I(–) [i.e., CsPb(Br:Cl)(3) or CsPb(Br:I)(3)]. In this work, we p...

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Autores principales: Akkerman, Quinten A., Bladt, Eva, Petralanda, Urko, Dang, Zhiya, Sartori, Emanuela, Baranov, Dmitry, Abdelhady, Ahmed L., Infante, Ivan, Bals, Sara, Manna, Liberato
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2019
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7497717/
https://www.ncbi.nlm.nih.gov/pubmed/32952295
http://dx.doi.org/10.1021/acs.chemmater.9b00489
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author Akkerman, Quinten A.
Bladt, Eva
Petralanda, Urko
Dang, Zhiya
Sartori, Emanuela
Baranov, Dmitry
Abdelhady, Ahmed L.
Infante, Ivan
Bals, Sara
Manna, Liberato
author_facet Akkerman, Quinten A.
Bladt, Eva
Petralanda, Urko
Dang, Zhiya
Sartori, Emanuela
Baranov, Dmitry
Abdelhady, Ahmed L.
Infante, Ivan
Bals, Sara
Manna, Liberato
author_sort Akkerman, Quinten A.
collection PubMed
description [Image: see text] The vast majority of lead halide perovskite (LHP) nanocrystals (NCs) are currently based on either a single halide composition (CsPbCl(3), CsPbBr(3), and CsPbI(3)) or an alloyed mixture of bromide with either Cl(–) or I(–) [i.e., CsPb(Br:Cl)(3) or CsPb(Br:I)(3)]. In this work, we present the synthesis as well as a detailed optical and structural study of two halide alloying cases that have not previously been reported for LHP NCs: Cs(2)PbI(2)Cl(2) NCs and triple halide CsPb(Cl:Br:I)(3) NCs. In the case of Cs(2)PbI(2)Cl(2), we observe for the first time NCs with a fully inorganic Ruddlesden–Popper phase (RPP) crystal structure. Unlike the well-explored organic–inorganic RPP, here, the RPP formation is triggered by the size difference between the halide ions. These NCs exhibit a strong excitonic absorption, albeit with a weak photoluminescence quantum yield (PLQY). In the case of the triple halide CsPb(Cl:Br:I)(3) composition, the NCs comprise a CsPbBr(2)Cl perovskite crystal lattice with only a small amount of incorporated iodide, which segregates at RPP planes’ interfaces within the CsPb(Cl:Br:I)(3) NCs. Supported by density functional theory calculations and postsynthetic surface treatments to enhance the PLQY, we show that the combination of iodide segregation and defective RPP interfaces are most likely linked to the strong PL quenching observed in these nanostructures. In summary, this work demonstrates the limits of halide alloying in LHP NCs because a mixture that contains halide ions of very different sizes leads to the formation of defective RPP interfaces and a severe quenching of LHP NC’s optical properties.
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spelling pubmed-74977172020-09-18 Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals Akkerman, Quinten A. Bladt, Eva Petralanda, Urko Dang, Zhiya Sartori, Emanuela Baranov, Dmitry Abdelhady, Ahmed L. Infante, Ivan Bals, Sara Manna, Liberato Chem Mater [Image: see text] The vast majority of lead halide perovskite (LHP) nanocrystals (NCs) are currently based on either a single halide composition (CsPbCl(3), CsPbBr(3), and CsPbI(3)) or an alloyed mixture of bromide with either Cl(–) or I(–) [i.e., CsPb(Br:Cl)(3) or CsPb(Br:I)(3)]. In this work, we present the synthesis as well as a detailed optical and structural study of two halide alloying cases that have not previously been reported for LHP NCs: Cs(2)PbI(2)Cl(2) NCs and triple halide CsPb(Cl:Br:I)(3) NCs. In the case of Cs(2)PbI(2)Cl(2), we observe for the first time NCs with a fully inorganic Ruddlesden–Popper phase (RPP) crystal structure. Unlike the well-explored organic–inorganic RPP, here, the RPP formation is triggered by the size difference between the halide ions. These NCs exhibit a strong excitonic absorption, albeit with a weak photoluminescence quantum yield (PLQY). In the case of the triple halide CsPb(Cl:Br:I)(3) composition, the NCs comprise a CsPbBr(2)Cl perovskite crystal lattice with only a small amount of incorporated iodide, which segregates at RPP planes’ interfaces within the CsPb(Cl:Br:I)(3) NCs. Supported by density functional theory calculations and postsynthetic surface treatments to enhance the PLQY, we show that the combination of iodide segregation and defective RPP interfaces are most likely linked to the strong PL quenching observed in these nanostructures. In summary, this work demonstrates the limits of halide alloying in LHP NCs because a mixture that contains halide ions of very different sizes leads to the formation of defective RPP interfaces and a severe quenching of LHP NC’s optical properties. American Chemical Society 2019-03-04 2019-03-26 /pmc/articles/PMC7497717/ /pubmed/32952295 http://dx.doi.org/10.1021/acs.chemmater.9b00489 Text en Copyright © 2019 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Akkerman, Quinten A.
Bladt, Eva
Petralanda, Urko
Dang, Zhiya
Sartori, Emanuela
Baranov, Dmitry
Abdelhady, Ahmed L.
Infante, Ivan
Bals, Sara
Manna, Liberato
Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals
title Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals
title_full Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals
title_fullStr Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals
title_full_unstemmed Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals
title_short Fully Inorganic Ruddlesden–Popper Double Cl–I and Triple Cl–Br–I Lead Halide Perovskite Nanocrystals
title_sort fully inorganic ruddlesden–popper double cl–i and triple cl–br–i lead halide perovskite nanocrystals
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7497717/
https://www.ncbi.nlm.nih.gov/pubmed/32952295
http://dx.doi.org/10.1021/acs.chemmater.9b00489
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