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Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity

[Image: see text] Halide mixing is one of the most powerful techniques to tune the optical bandgap of metal-halide perovskites. However, halide mixing has commonly been observed to result in phase segregation, which reduces excited-state transport and limits device performance. While the current emp...

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Autores principales: Seitz, Michael, Meléndez, Marc, York, Peyton, Kurtz, Daniel A., Magdaleno, Alvaro J., Alcázar-Cano, Nerea, Kshirsagar, Anuraj S., Gangishetty, Mahesh K., Delgado-Buscalioni, Rafael, Congreve, Daniel N., Prins, Ferry
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8762701/
https://www.ncbi.nlm.nih.gov/pubmed/35059502
http://dx.doi.org/10.1021/acsenergylett.1c02403
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author Seitz, Michael
Meléndez, Marc
York, Peyton
Kurtz, Daniel A.
Magdaleno, Alvaro J.
Alcázar-Cano, Nerea
Kshirsagar, Anuraj S.
Gangishetty, Mahesh K.
Delgado-Buscalioni, Rafael
Congreve, Daniel N.
Prins, Ferry
author_facet Seitz, Michael
Meléndez, Marc
York, Peyton
Kurtz, Daniel A.
Magdaleno, Alvaro J.
Alcázar-Cano, Nerea
Kshirsagar, Anuraj S.
Gangishetty, Mahesh K.
Delgado-Buscalioni, Rafael
Congreve, Daniel N.
Prins, Ferry
author_sort Seitz, Michael
collection PubMed
description [Image: see text] Halide mixing is one of the most powerful techniques to tune the optical bandgap of metal-halide perovskites. However, halide mixing has commonly been observed to result in phase segregation, which reduces excited-state transport and limits device performance. While the current emphasis lies on the development of strategies to prevent phase segregation, it remains unclear how halide mixing may affect excited-state transport even if phase purity is maintained. Here, we study exciton transport in phase pure mixed-halide 2D perovskites of (PEA)(2)Pb(I(1–x)Br(x))(4). Using transient photoluminescence microscopy, we show that, despite phase purity, halide mixing inhibits exciton transport. We find a significant reduction even for relatively low alloying concentrations. By performing Brownian dynamics simulations, we are able to reproduce our experimental results and attribute the decrease in diffusivity to the energetically disordered potential landscape that arises due to the intrinsic random distribution of alloying sites.
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spelling pubmed-87627012022-01-18 Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity Seitz, Michael Meléndez, Marc York, Peyton Kurtz, Daniel A. Magdaleno, Alvaro J. Alcázar-Cano, Nerea Kshirsagar, Anuraj S. Gangishetty, Mahesh K. Delgado-Buscalioni, Rafael Congreve, Daniel N. Prins, Ferry ACS Energy Lett [Image: see text] Halide mixing is one of the most powerful techniques to tune the optical bandgap of metal-halide perovskites. However, halide mixing has commonly been observed to result in phase segregation, which reduces excited-state transport and limits device performance. While the current emphasis lies on the development of strategies to prevent phase segregation, it remains unclear how halide mixing may affect excited-state transport even if phase purity is maintained. Here, we study exciton transport in phase pure mixed-halide 2D perovskites of (PEA)(2)Pb(I(1–x)Br(x))(4). Using transient photoluminescence microscopy, we show that, despite phase purity, halide mixing inhibits exciton transport. We find a significant reduction even for relatively low alloying concentrations. By performing Brownian dynamics simulations, we are able to reproduce our experimental results and attribute the decrease in diffusivity to the energetically disordered potential landscape that arises due to the intrinsic random distribution of alloying sites. American Chemical Society 2021-12-22 2022-01-14 /pmc/articles/PMC8762701/ /pubmed/35059502 http://dx.doi.org/10.1021/acsenergylett.1c02403 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Seitz, Michael
Meléndez, Marc
York, Peyton
Kurtz, Daniel A.
Magdaleno, Alvaro J.
Alcázar-Cano, Nerea
Kshirsagar, Anuraj S.
Gangishetty, Mahesh K.
Delgado-Buscalioni, Rafael
Congreve, Daniel N.
Prins, Ferry
Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity
title Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity
title_full Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity
title_fullStr Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity
title_full_unstemmed Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity
title_short Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity
title_sort halide mixing inhibits exciton transport in two-dimensional perovskites despite phase purity
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8762701/
https://www.ncbi.nlm.nih.gov/pubmed/35059502
http://dx.doi.org/10.1021/acsenergylett.1c02403
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