Cover Image

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

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 s...

Full description

Saved in:
Bibliographic Details
Main Authors: Ding, Thomas (Author) , Ott, Christian (Author) , Kaldun, Andreas (Author) , Blättermann, Alexander (Author) , Meyer, Kristina (Author) , Stooß, Veit (Author) , Rebholz, Marc (Author) , Birk, Paul (Author) , Hartmann, Maximilian (Author) , Brown, Andrew (Author) , Hart, Hugo Van Der (Author) , Pfeifer, Thomas (Author)
Format: Article (Journal) Editorial
Language:English
Published: 5 January 2016
In: Optics letters
Year: 2016, Volume: 41, Issue: 4, Pages: 709-712
ISSN:1539-4794
DOI:10.1364/OL.41.000709
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1364/OL.41.000709
Verlag, lizenzpflichtig, Volltext: https://www.osapublishing.org/ol/abstract.cfm?uri=ol-41-4-709
Get full text
Author Notes:Thomas Ding, Christian Ott, Andreas Kaldun, Alexander Blättermann, Kristina Meyer, Veit Stooss, Marc Rebholz, Paul Birk, Maximilian Hartmann, Andrew Brown, Hugo Van Der Hart, and Thomas Pfeifer
Description
Summary: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.
Item Description:Gesehen am 08.05.2020
Physical Description:Online Resource
ISSN:1539-4794
DOI:10.1364/OL.41.000709

Similar Items