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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...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical
Society
2019
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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. |
format | Online Article Text |
id | pubmed-7497717 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | American Chemical
Society |
record_format | MEDLINE/PubMed |
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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