Cargando…

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...

Descripción completa

Detalles Bibliográficos
Autores principales: 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
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
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
_version_ 1785033073522376704
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
work_keys_str_mv AT laitzmadeleine uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT kaplanalexanderek uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT deschampsjude uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT barotovulugbek uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT proppeandrewh uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT garciabenitoines uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT osherovanna uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT grancinigiulia uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT dequilettesdanew uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT nelsonkeitha uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT bawendimoungig uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites
AT bulovicvladimir uncoveringtemperaturedependentexcitonpolaritonrelaxationmechanismsinhybridorganicinorganicperovskites