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

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

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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, [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.",

author = "A. Ferr{\'e} and Boguslavskiy, {A. E.} and M. Dagan and V. Blanchet and Bruner, {B. D.} and F. Burgy and A. Camper and D. Descamps and B. Fabre and N. Fedorov and J. Gaudin and G. Geoffroy and J. Mikosch and S. Patchkovskii and S. Petit and T. Ruchon and H. Soifer and D. Staedter and I. Wilkinson and A. Stolow and N. Dudovich and Y. Mairesse",

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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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T1 - Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

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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