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Driving chemical reactions with polariton condensates

When molecular transitions strongly couple to photon modes, they form hybrid light-matter modes called polaritons. Collective vibrational strong coupling is a promising avenue for control of chemistry, but this can be deterred by the large number of quasi-degenerate dark modes. The macroscopic occup...

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Autores principales: Pannir-Sivajothi, Sindhana, Campos-Gonzalez-Angulo, Jorge A., Martínez-Martínez, Luis A., Sinha, Shubham, Yuen-Zhou, Joel
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8960839/
https://www.ncbi.nlm.nih.gov/pubmed/35347131
http://dx.doi.org/10.1038/s41467-022-29290-9
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author Pannir-Sivajothi, Sindhana
Campos-Gonzalez-Angulo, Jorge A.
Martínez-Martínez, Luis A.
Sinha, Shubham
Yuen-Zhou, Joel
author_facet Pannir-Sivajothi, Sindhana
Campos-Gonzalez-Angulo, Jorge A.
Martínez-Martínez, Luis A.
Sinha, Shubham
Yuen-Zhou, Joel
author_sort Pannir-Sivajothi, Sindhana
collection PubMed
description When molecular transitions strongly couple to photon modes, they form hybrid light-matter modes called polaritons. Collective vibrational strong coupling is a promising avenue for control of chemistry, but this can be deterred by the large number of quasi-degenerate dark modes. The macroscopic occupation of a single polariton mode by excitations, as observed in Bose-Einstein condensation, offers promise for overcoming this issue. Here we theoretically investigate the effect of vibrational polariton condensation on the kinetics of electron transfer processes. Compared with excitation with infrared laser sources, the vibrational polariton condensate changes the reaction yield significantly at room temperature due to additional channels with reduced activation barriers resulting from the large accumulation of energy in the lower polariton, and the many modes available for energy redistribution during the reaction. Our results offer tantalizing opportunities to use condensates for driving chemical reactions, kinetically bypassing usual constraints of fast intramolecular vibrational redistribution in condensed phase.
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spelling pubmed-89608392022-04-20 Driving chemical reactions with polariton condensates Pannir-Sivajothi, Sindhana Campos-Gonzalez-Angulo, Jorge A. Martínez-Martínez, Luis A. Sinha, Shubham Yuen-Zhou, Joel Nat Commun Article When molecular transitions strongly couple to photon modes, they form hybrid light-matter modes called polaritons. Collective vibrational strong coupling is a promising avenue for control of chemistry, but this can be deterred by the large number of quasi-degenerate dark modes. The macroscopic occupation of a single polariton mode by excitations, as observed in Bose-Einstein condensation, offers promise for overcoming this issue. Here we theoretically investigate the effect of vibrational polariton condensation on the kinetics of electron transfer processes. Compared with excitation with infrared laser sources, the vibrational polariton condensate changes the reaction yield significantly at room temperature due to additional channels with reduced activation barriers resulting from the large accumulation of energy in the lower polariton, and the many modes available for energy redistribution during the reaction. Our results offer tantalizing opportunities to use condensates for driving chemical reactions, kinetically bypassing usual constraints of fast intramolecular vibrational redistribution in condensed phase. Nature Publishing Group UK 2022-03-28 /pmc/articles/PMC8960839/ /pubmed/35347131 http://dx.doi.org/10.1038/s41467-022-29290-9 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
Pannir-Sivajothi, Sindhana
Campos-Gonzalez-Angulo, Jorge A.
Martínez-Martínez, Luis A.
Sinha, Shubham
Yuen-Zhou, Joel
Driving chemical reactions with polariton condensates
title Driving chemical reactions with polariton condensates
title_full Driving chemical reactions with polariton condensates
title_fullStr Driving chemical reactions with polariton condensates
title_full_unstemmed Driving chemical reactions with polariton condensates
title_short Driving chemical reactions with polariton condensates
title_sort driving chemical reactions with polariton condensates
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8960839/
https://www.ncbi.nlm.nih.gov/pubmed/35347131
http://dx.doi.org/10.1038/s41467-022-29290-9
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