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Volume 194, 2016
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Multidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields

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Abstract

High harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.

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Publication details

The article was received on 11 May 2016, accepted on 07 Jul 2016 and first published on 26 Sep 2016


Article type: Paper
DOI: 10.1039/C6FD00130K
Citation: Faraday Discuss., 2016,194, 369-405
  • Open access: Creative Commons BY-NC license
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    Multidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields

    B. D. Bruner, Z. Mašín, M. Negro, F. Morales, D. Brambila, M. Devetta, D. Faccialà, A. G. Harvey, M. Ivanov, Y. Mairesse, S. Patchkovskii, V. Serbinenko, H. Soifer, S. Stagira, C. Vozzi, N. Dudovich and O. Smirnova, Faraday Discuss., 2016, 194, 369
    DOI: 10.1039/C6FD00130K

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