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

Research output: Contribution to journalArticle

24 Citations (Scopus)
489 Downloads (Pure)

Abstract

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
Volume41
Issue number4
Early online date07 Jan 2016
DOIs
Publication statusPublished - 15 Feb 2016

Keywords

  • Attosecond
  • spectroscopy
  • AB-INITIO
  • R-MATRIX METHOD

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  • Datasets

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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

    Activity: Participating in or organising an event typesParticipation in workshop, seminar, course

    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