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Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal ap...

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Autores principales: Ferré, A., Boguslavskiy, A. E., Dagan, M., Blanchet, V., Bruner, B. D., Burgy, F., Camper, A., Descamps, D., Fabre, B., Fedorov, N., Gaudin, J., Geoffroy, G., Mikosch, J., Patchkovskii, S., Petit, S., Ruchon, T., Soifer, H., Staedter, D., Wilkinson, I., Stolow, A., Dudovich, N., Mairesse, Y.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Pub. Group 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4354235/
https://www.ncbi.nlm.nih.gov/pubmed/25608712
http://dx.doi.org/10.1038/ncomms6952
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author Ferré, A.
Boguslavskiy, A. E.
Dagan, M.
Blanchet, V.
Bruner, B. D.
Burgy, F.
Camper, A.
Descamps, D.
Fabre, B.
Fedorov, N.
Gaudin, J.
Geoffroy, G.
Mikosch, J.
Patchkovskii, S.
Petit, S.
Ruchon, T.
Soifer, H.
Staedter, D.
Wilkinson, I.
Stolow, A.
Dudovich, N.
Mairesse, Y.
author_facet Ferré, A.
Boguslavskiy, A. E.
Dagan, M.
Blanchet, V.
Bruner, B. D.
Burgy, F.
Camper, A.
Descamps, D.
Fabre, B.
Fedorov, N.
Gaudin, J.
Geoffroy, G.
Mikosch, J.
Patchkovskii, S.
Petit, S.
Ruchon, T.
Soifer, H.
Staedter, D.
Wilkinson, I.
Stolow, A.
Dudovich, N.
Mairesse, Y.
author_sort Ferré, A.
collection PubMed
description High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF(6) as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20–26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.
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spelling pubmed-43542352015-03-20 Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation Ferré, A. Boguslavskiy, A. E. Dagan, M. Blanchet, V. Bruner, B. D. Burgy, F. Camper, A. Descamps, D. Fabre, B. Fedorov, N. Gaudin, J. Geoffroy, G. Mikosch, J. Patchkovskii, S. Petit, S. Ruchon, T. Soifer, H. Staedter, D. Wilkinson, I. Stolow, A. Dudovich, N. Mairesse, Y. Nat Commun Article High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF(6) as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20–26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected. Nature Pub. Group 2015-01-22 /pmc/articles/PMC4354235/ /pubmed/25608712 http://dx.doi.org/10.1038/ncomms6952 Text en Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved. http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
spellingShingle Article
Ferré, A.
Boguslavskiy, A. E.
Dagan, M.
Blanchet, V.
Bruner, B. D.
Burgy, F.
Camper, A.
Descamps, D.
Fabre, B.
Fedorov, N.
Gaudin, J.
Geoffroy, G.
Mikosch, J.
Patchkovskii, S.
Petit, S.
Ruchon, T.
Soifer, H.
Staedter, D.
Wilkinson, I.
Stolow, A.
Dudovich, N.
Mairesse, Y.
Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
title Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
title_full Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
title_fullStr Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
title_full_unstemmed Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
title_short Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
title_sort multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4354235/
https://www.ncbi.nlm.nih.gov/pubmed/25608712
http://dx.doi.org/10.1038/ncomms6952
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