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Journal Article

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

MPS-Authors
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Ding,  Thomas
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Ott,  Christian
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

/persons/resource/persons37846

Kaldun,  Andreas
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Blättermann,  Alexander
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Meyer,  Kristina
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Stooß,  Veit
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Rebholz,  M.
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Birk,  Paul
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Hartmann,  Maximilian
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

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Pfeifer,  Thomas
Division Prof. Dr. Thomas Pfeifer, MPI for Nuclear Physics, Max Planck Society;

External Resource

https://www.osapublishing.org/ol/abstract.cfm?uri=ol-41-4-709
(Publisher version)

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Fulltext (public)

1510.08698v1
(Preprint), 790KB

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Citation

Ding, T., Ott, C., Kaldun, A., Blättermann, A., Meyer, K., Stooß, V., et al. (2016). Time-resolved four-wave-mixing spectroscopy for inner-valence transitions. Optics Letters, 41(4), 709-712. doi:10.1364/OL.41.000709.


Cite as: https://hdl.handle.net/11858/00-001M-0000-002B-1EED-B
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.