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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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Formato: | Online Artículo Texto |
Lenguaje: | English |
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Nature Publishing Group UK
2022
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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. |
format | Online Article Text |
id | pubmed-9814737 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
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 |
work_keys_str_mv | AT ribeiroraphaelf multimodepolaritoneffectsonmolecularenergytransportandspectralfluctuations |