Time-resolved four-wave-mixing spectroscopy for inner-valence transitions

Thomas Ding, Christian Ott, Andreas Kaldun, Alexander Blatterman, Kristina Meyer, Veit Stooss, Marc Rebholz, Paul Birk, Maximilian Hartmann, Andrew Brown, Hugo Van Der Hart, Thomas Pfeifer

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Noncollinear four-wave-mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between spatially localized inner-valence transitions among different sites of a molecule in the extreme ultraviolet (XUV) spectral range have not been observed yet. As an experimental step toward this goal, we perform time-resolved FWM spectroscopy with femtosecond NIR and attosecond XUV pulses. The first two pulses (XUV-NIR) coincide in time and act as coherent excitation fields, while the third pulse (NIR) acts as a probe. As a first application, we show how coupling dynamics between odd- and even-parity, inner-valence excited states of neon can be revealed using a two-dimensional spectral representation. Experimentally obtained results are found to be in good agreement with ab initio time-dependent R-matrix calculations providing the full description of multielectron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.
Original languageEnglish
Pages (from-to)709-712
Number of pages4
JournalOptics Letters
Issue number4
Early online date07 Jan 2016
Publication statusPublished - 15 Feb 2016


  • Attosecond
  • spectroscopy

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    • 1 Participation in conference
    • 1 Participation in workshop, seminar, course

    Faraday discussion: Ultrafast imaging and photochemical dynamics

    Andrew Brown (Participant)

    31 Aug 201602 Sep 2016

    Activity: Participating in or organising an event typesParticipation in conference

    Bothe Colloquium

    Andrew Brown (Invited speaker)

    13 May 2015

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    Cite this

    Ding, T., Ott, C., Kaldun, A., Blatterman, A., Meyer, K., Stooss, V., Rebholz, M., Birk, P., Hartmann, M., Brown, A., Van Der Hart, H., & Pfeifer, T. (2016). Time-resolved four-wave-mixing spectroscopy for inner-valence transitions. Optics Letters, 41(4), 709-712. https://doi.org/10.1364/OL.41.000709