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Ultrafast imaging of polariton propagation and interactions

Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated i...

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Autores principales: Xu, Ding, Mandal, Arkajit, Baxter, James M., Cheng, Shan-Wen, Lee, Inki, Su, Haowen, Liu, Song, Reichman, David R., Delor, Milan
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10313693/
https://www.ncbi.nlm.nih.gov/pubmed/37391396
http://dx.doi.org/10.1038/s41467-023-39550-x
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author Xu, Ding
Mandal, Arkajit
Baxter, James M.
Cheng, Shan-Wen
Lee, Inki
Su, Haowen
Liu, Song
Reichman, David R.
Delor, Milan
author_facet Xu, Ding
Mandal, Arkajit
Baxter, James M.
Cheng, Shan-Wen
Lee, Inki
Su, Haowen
Liu, Song
Reichman, David R.
Delor, Milan
author_sort Xu, Ding
collection PubMed
description Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP–phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP–phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions.
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spelling pubmed-103136932023-07-02 Ultrafast imaging of polariton propagation and interactions Xu, Ding Mandal, Arkajit Baxter, James M. Cheng, Shan-Wen Lee, Inki Su, Haowen Liu, Song Reichman, David R. Delor, Milan Nat Commun Article Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP–phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP–phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions. Nature Publishing Group UK 2023-06-30 /pmc/articles/PMC10313693/ /pubmed/37391396 http://dx.doi.org/10.1038/s41467-023-39550-x 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 licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence 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 licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Xu, Ding
Mandal, Arkajit
Baxter, James M.
Cheng, Shan-Wen
Lee, Inki
Su, Haowen
Liu, Song
Reichman, David R.
Delor, Milan
Ultrafast imaging of polariton propagation and interactions
title Ultrafast imaging of polariton propagation and interactions
title_full Ultrafast imaging of polariton propagation and interactions
title_fullStr Ultrafast imaging of polariton propagation and interactions
title_full_unstemmed Ultrafast imaging of polariton propagation and interactions
title_short Ultrafast imaging of polariton propagation and interactions
title_sort ultrafast imaging of polariton propagation and interactions
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10313693/
https://www.ncbi.nlm.nih.gov/pubmed/37391396
http://dx.doi.org/10.1038/s41467-023-39550-x
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