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Multimode polariton effects on molecular energy transport and spectral fluctuations

Despite the potential paradigm breaking capability of microcavities to control chemical processes, the extent to which photonic devices change properties of molecular materials is still unclear, in part due to challenges in modeling hybrid light-matter excitations delocalized over many length scales...

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Autor principal: Ribeiro, Raphael F.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814737/
https://www.ncbi.nlm.nih.gov/pubmed/36697846
http://dx.doi.org/10.1038/s42004-022-00660-0
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author Ribeiro, Raphael F.
author_facet Ribeiro, Raphael F.
author_sort Ribeiro, Raphael F.
collection PubMed
description Despite the potential paradigm breaking capability of microcavities to control chemical processes, the extent to which photonic devices change properties of molecular materials is still unclear, in part due to challenges in modeling hybrid light-matter excitations delocalized over many length scales. We overcome these challenges for a photonic wire under strong coupling with a molecular ensemble. Our simulations provide a detailed picture of the effect of photonic wires on spectral and transport properties of a disordered molecular material. We find stronger changes to the probed molecular observables when the cavity is redshifted relative to the molecules and energetic disorder is weak. These trends are expected to hold also in higher-dimensional cavities, but are not captured with theories that only include a single cavity-mode. Therefore, our results raise important issues for future experiments and model building focused on unraveling new ways to manipulate chemistry with optical cavities.
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spelling pubmed-98147372023-01-10 Multimode polariton effects on molecular energy transport and spectral fluctuations Ribeiro, Raphael F. Commun Chem Article Despite the potential paradigm breaking capability of microcavities to control chemical processes, the extent to which photonic devices change properties of molecular materials is still unclear, in part due to challenges in modeling hybrid light-matter excitations delocalized over many length scales. We overcome these challenges for a photonic wire under strong coupling with a molecular ensemble. Our simulations provide a detailed picture of the effect of photonic wires on spectral and transport properties of a disordered molecular material. We find stronger changes to the probed molecular observables when the cavity is redshifted relative to the molecules and energetic disorder is weak. These trends are expected to hold also in higher-dimensional cavities, but are not captured with theories that only include a single cavity-mode. Therefore, our results raise important issues for future experiments and model building focused on unraveling new ways to manipulate chemistry with optical cavities. Nature Publishing Group UK 2022-04-06 /pmc/articles/PMC9814737/ /pubmed/36697846 http://dx.doi.org/10.1038/s42004-022-00660-0 Text en © The Author(s) 2022 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
Ribeiro, Raphael F.
Multimode polariton effects on molecular energy transport and spectral fluctuations
title Multimode polariton effects on molecular energy transport and spectral fluctuations
title_full Multimode polariton effects on molecular energy transport and spectral fluctuations
title_fullStr Multimode polariton effects on molecular energy transport and spectral fluctuations
title_full_unstemmed Multimode polariton effects on molecular energy transport and spectral fluctuations
title_short Multimode polariton effects on molecular energy transport and spectral fluctuations
title_sort multimode polariton effects on molecular energy transport and spectral fluctuations
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9814737/
https://www.ncbi.nlm.nih.gov/pubmed/36697846
http://dx.doi.org/10.1038/s42004-022-00660-0
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