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Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses
Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a molecular wavepacket. A subsequent probe pulse can then dissociate or ionize the molecule, and measurement of the molecular f...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7078293/ https://www.ncbi.nlm.nih.gov/pubmed/32184408 http://dx.doi.org/10.1038/s41467-020-15196-x |
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author | Silva, R. E. F. Pino, Javier del García-Vidal, Francisco J. Feist, Johannes |
author_facet | Silva, R. E. F. Pino, Javier del García-Vidal, Francisco J. Feist, Johannes |
author_sort | Silva, R. E. F. |
collection | PubMed |
description | Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a molecular wavepacket. A subsequent probe pulse can then dissociate or ionize the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. Here, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light–matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light–matter) potentials in the strong light–matter coupling regime and bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a route towards ultrafast molecular spectroscopy with plasmonic nanocavities. |
format | Online Article Text |
id | pubmed-7078293 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-70782932020-03-19 Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses Silva, R. E. F. Pino, Javier del García-Vidal, Francisco J. Feist, Johannes Nat Commun Article Conventional approaches to probing ultrafast molecular dynamics rely on the use of synchronized laser pulses with a well-defined time delay. Typically, a pump pulse excites a molecular wavepacket. A subsequent probe pulse can then dissociate or ionize the molecule, and measurement of the molecular fragments provides information about where the wavepacket was for each time delay. Here, we propose to exploit the ultrafast nuclear-position-dependent emission obtained due to large light–matter coupling in plasmonic nanocavities to image wavepacket dynamics using only a single pump pulse. We show that the time-resolved emission from the cavity provides information about when the wavepacket passes a given region in nuclear configuration space. This approach can image both cavity-modified dynamics on polaritonic (hybrid light–matter) potentials in the strong light–matter coupling regime and bare-molecule dynamics in the intermediate coupling regime of large Purcell enhancements, and provides a route towards ultrafast molecular spectroscopy with plasmonic nanocavities. Nature Publishing Group UK 2020-03-17 /pmc/articles/PMC7078293/ /pubmed/32184408 http://dx.doi.org/10.1038/s41467-020-15196-x Text en © The Author(s) 2020 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/. |
spellingShingle | Article Silva, R. E. F. Pino, Javier del García-Vidal, Francisco J. Feist, Johannes Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
title | Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
title_full | Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
title_fullStr | Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
title_full_unstemmed | Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
title_short | Polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
title_sort | polaritonic molecular clock for all-optical ultrafast imaging of wavepacket dynamics without probe pulses |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7078293/ https://www.ncbi.nlm.nih.gov/pubmed/32184408 http://dx.doi.org/10.1038/s41467-020-15196-x |
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