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Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites
Hybrid perovskites have emerged as a promising material candidate for exciton-polariton (polariton) optoelectronics. Thermodynamically, low-threshold Bose-Einstein condensation requires efficient scattering to the polariton energy dispersion minimum, and many applications demand precise control of p...
Autores principales: | , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10140020/ https://www.ncbi.nlm.nih.gov/pubmed/37105984 http://dx.doi.org/10.1038/s41467-023-37772-7 |
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author | Laitz, Madeleine Kaplan, Alexander E. K. Deschamps, Jude Barotov, Ulugbek Proppe, Andrew H. García-Benito, Inés Osherov, Anna Grancini, Giulia deQuilettes, Dane W. Nelson, Keith A. Bawendi, Moungi G. Bulović, Vladimir |
author_facet | Laitz, Madeleine Kaplan, Alexander E. K. Deschamps, Jude Barotov, Ulugbek Proppe, Andrew H. García-Benito, Inés Osherov, Anna Grancini, Giulia deQuilettes, Dane W. Nelson, Keith A. Bawendi, Moungi G. Bulović, Vladimir |
author_sort | Laitz, Madeleine |
collection | PubMed |
description | Hybrid perovskites have emerged as a promising material candidate for exciton-polariton (polariton) optoelectronics. Thermodynamically, low-threshold Bose-Einstein condensation requires efficient scattering to the polariton energy dispersion minimum, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear. In this work, we perform temperature-dependent measurements of polaritons in low-dimensional perovskite wedged microcavities achieving a Rabi splitting of [Formula: see text] = 260 ± 5 meV. We change the Hopfield coefficients by moving the optical excitation along the cavity wedge and thus tune the strength of the primary polariton relaxation mechanisms in this material. We observe the polariton bottleneck regime and show that it can be overcome by harnessing the interplay between the different excitonic species whose corresponding dynamics are modified by strong coupling. This work provides an understanding of polariton relaxation in perovskites benefiting from efficient, material-specific relaxation pathways and intracavity pumping schemes from thermally brightened excitonic species. |
format | Online Article Text |
id | pubmed-10140020 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-101400202023-04-29 Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites Laitz, Madeleine Kaplan, Alexander E. K. Deschamps, Jude Barotov, Ulugbek Proppe, Andrew H. García-Benito, Inés Osherov, Anna Grancini, Giulia deQuilettes, Dane W. Nelson, Keith A. Bawendi, Moungi G. Bulović, Vladimir Nat Commun Article Hybrid perovskites have emerged as a promising material candidate for exciton-polariton (polariton) optoelectronics. Thermodynamically, low-threshold Bose-Einstein condensation requires efficient scattering to the polariton energy dispersion minimum, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear. In this work, we perform temperature-dependent measurements of polaritons in low-dimensional perovskite wedged microcavities achieving a Rabi splitting of [Formula: see text] = 260 ± 5 meV. We change the Hopfield coefficients by moving the optical excitation along the cavity wedge and thus tune the strength of the primary polariton relaxation mechanisms in this material. We observe the polariton bottleneck regime and show that it can be overcome by harnessing the interplay between the different excitonic species whose corresponding dynamics are modified by strong coupling. This work provides an understanding of polariton relaxation in perovskites benefiting from efficient, material-specific relaxation pathways and intracavity pumping schemes from thermally brightened excitonic species. Nature Publishing Group UK 2023-04-27 /pmc/articles/PMC10140020/ /pubmed/37105984 http://dx.doi.org/10.1038/s41467-023-37772-7 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Laitz, Madeleine Kaplan, Alexander E. K. Deschamps, Jude Barotov, Ulugbek Proppe, Andrew H. García-Benito, Inés Osherov, Anna Grancini, Giulia deQuilettes, Dane W. Nelson, Keith A. Bawendi, Moungi G. Bulović, Vladimir Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
title | Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
title_full | Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
title_fullStr | Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
title_full_unstemmed | Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
title_short | Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
title_sort | uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10140020/ https://www.ncbi.nlm.nih.gov/pubmed/37105984 http://dx.doi.org/10.1038/s41467-023-37772-7 |
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