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Time-resolved Four-wave-mixing Spectroscopy for Inner-valence Transitions by Ding, Thomas; Ott, Christian; Kaldun, Andreas; Blättermann, Alexander; Meyer, Kristina; Stooß, Veit; Rebholz, Marc; Birk, Paul; Hartmann, Maximilian; Brown, Andrew; Van Der Hart, Hugo; Pfeifer, Thomas is a scholarly article available to read on EtoBox.

What is Time-resolved Four-wave-mixing Spectroscopy for Inner-valence Transitions about?

Non-collinear 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 towards 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 multi-electron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.

Author

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

Published

2015

Language

EN