Multi-channel Electronic and Vibrational Dynamics in Polyatomic High-order Harmonic Generation
Abstract
High-order harmonic generation in polyatomic molecules generally involves multiple channels, each associated with a different orbital. Their unambiguous assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach, using unaligned SF molecules as an example, where we combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Channel-resolved above-threshold ionization measurements reveal that strong-field ionization opens four channels. Two of them, identified by monitoring the ellipticity dependence of the high-harmonic emission, are found to dominate the harmonic signal. A switch from the HOMO-3 to the HOMO-1 channel at 26 eV is confirmed by a phase jump in the harmonic emission, and by the differing dynamical responses to molecular vibrations. This study demonstrates a modus operandi for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.
Cite
@article{arxiv.1407.6213,
title = {Multi-channel Electronic and Vibrational Dynamics in Polyatomic High-order Harmonic Generation},
author = {A. Ferré and A. E. Boguslavskiy and M. Dagan and V. Blanchet and B. Bruner 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},
journal= {arXiv preprint arXiv:1407.6213},
year = {2015}
}
Comments
10 pages, 7 figures