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

A. Ferré; A. E. Boguslavskiy; M. Dagan; V. Blanchet; B. D. Bruner; F. Burgy; A. Camper; D. Descamps; B. Fabre; N. Fedorov; J. Gaudin; G. Geoffroy; J. Mikosch; S. Patchkovskii; S. Petit; T. Ruchon; H. Soifer; D. Staedter; I. Wilkinson; A. Stolow; N. Dudovich; Y. Mairesse

doi:10.1038/ncomms6952

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

A. Ferré, A. E. Boguslavskiy, M. Dagan, V. Blanchet, B. D. Bruner, F. Burgy, A. Camper, D. Descamps, B. Fabre, N. Fedorov, J. Gaudin, G. Geoffroy, J. Mikosch, S. Patchkovskii, S. Petit, T. Ruchon, H. Soifer, D. Staedter, I. Wilkinson, A. StolowN. Dudovich, Y. Mairesse^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

74 Scopus citations

Abstract

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 SF₆ 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.

Original language	English
Article number	5952
Journal	Nature Communications
Volume	6
DOIs	https://doi.org/10.1038/ncomms6952
State	Published - 22 Jan 2015
Externally published	Yes

Funding

Funders	Funder number
l’Ambassade de France au Canada
Israel Science Foundation
Israeli Centers of Research Excellence program
European Commission
Natural Sciences and Engineering Research Council of Canada
Minerva Foundation
European Research Council
NSERC (Canada)
Crown Photonics Center
Agence Nationale de la Recherche	ANR-14-CE32-0014
l’Agence Nationale pour la Recherche	ANR-14-CE32-0014 MISFITS
Seventh Framework Programme	228334, 242334
Conseil Régional Aquitaine	20091304003, 2.1.3-09010502

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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., ... Mairesse, Y. (2015). Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation. Nature Communications, 6, Article 5952. https://doi.org/10.1038/ncomms6952

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title = "Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation",

abstract = "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 SF6 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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Ferré, A, Boguslavskiy, AE, Dagan, M, Blanchet, V, Bruner, BD, 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 2015, 'Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation', Nature Communications, vol. 6, 5952. https://doi.org/10.1038/ncomms6952

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AU - Ferré, A.

AU - Boguslavskiy, A. E.

AU - Dagan, M.

AU - Blanchet, V.

AU - Bruner, B. D.

AU - Burgy, F.

AU - Camper, A.

AU - Descamps, D.

AU - Fabre, B.

AU - Fedorov, N.

AU - Gaudin, J.

AU - Geoffroy, G.

AU - Mikosch, J.

AU - Patchkovskii, S.

AU - Petit, S.

AU - Ruchon, T.

AU - Soifer, H.

AU - Staedter, D.

AU - Wilkinson, I.

AU - Stolow, A.

AU - Dudovich, N.

AU - Mairesse, Y.

PY - 2015/1/22

Y1 - 2015/1/22

N2 - 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 SF6 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.

AB - 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 SF6 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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Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

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