XUV pump–XUV probe transient absorption spectroscopy at FELs

Thomas Ding; Marc Rebholz; Lennart Aufleger; Maximilian Hartmann; Veit Stooß; Alexander Magunia; Paul Birk; Gergana Dimitrova Borisova; Carina da Costa Castanheira; Patrick Rupprecht; Yonghao Mi; Thomas Gaumnitz; Zhi-Heng Loh; Sebastian Roling; Marco Butz; Helmut Zacharias; Stefan Düsterer; Rolf Treusch; Christian Ott; Thomas Pfeifer

doi:10.1039/D0FD00107D

XUV pump–XUV probe transient absorption spectroscopy at FELs

Thomas Ding,*^a Marc Rebholz,^a Lennart Aufleger,^a Maximilian Hartmann,

^a Veit Stooß,^a Alexander Magunia,^a Paul Birk,^a Gergana Dimitrova Borisova,^a Carina da Costa Castanheira,^a Patrick Rupprecht,

^a Yonghao Mi,

^a Thomas Gaumnitz,^b Zhi-Heng Loh,^c Sebastian Roling,^d Marco Butz,^e Helmut Zacharias,

^e Stefan Düsterer,^f Rolf Treusch,

^f Christian Ott

^a and Thomas Pfeifer

^a

Author affiliations

* Corresponding authors

^a Max-Planck-Institut für Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany
E-mail: christian.ott@mpi-hd.mpg.de, thomas.pfeifer@mpi-hd.mpg.de

^b Laboratorium für Physikalische Chemie, ETH Zürich, Vladimir-Prelog-Weg 2, 8093 Zürich, Switzerland

^c Division of Chemistry and Biological Chemistry, Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore

^d Physikalisches Institut der Westfälischen Wilhelms-Universität Münster, Wilhelm-Klemm-Straße 10, 48149 Münster, Germany

^e Center for Soft Nanoscience, Busso-Peuss-Straße 10, 48149 Münster, Germany

^f Deutsches Elektronen-Synchrotron DESY, Notkestraße 85, 22607 Hamburg, Germany

Abstract

The emergence of ultra-intense extreme-ultraviolet (XUV) and X-ray free-electron lasers (FELs) has opened the door for the experimental realization of non-linear XUV and X-ray spectroscopy techniques. Here we demonstrate an experimental setup for an all-XUV transient absorption spectroscopy method for gas-phase targets at the FEL. The setup combines a high spectral resolving power of E/ΔE ≈ 1500 with sub-femtosecond interferometric resolution, and covers a broad XUV photon-energy range between approximately 20 and 110 eV. We demonstrate the feasibility of this setup firstly on a neon target. Here, we intensity- and time-resolve key aspects of non-linear XUV-FEL light–matter interactions, namely the non-resonant ionization dynamics and resonant coupling dynamics of bound states, including XUV-induced Stark shifts of energy levels. Secondly, we show that this setup is capable of tracking the XUV-initiated dissociation dynamics of small molecular targets (oxygen and diiodomethane) with site-specific resolution, by measuring the XUV transient absorption spectrum. In general, benefitting from a single-shot detection capability, we show that the setup and method provides single-shot phase-locked XUV pulse pairs. This lays the foundation to perform, in the future, experiments as a function of the XUV interferometric time delay and the relative phase, which enables advanced coherent non-linear spectroscopy schemes in the XUV and X-ray spectral range.

This article is part of the themed collection: Time resolved imaging of photo-induced dynamics

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XUV pump–XUV probe transient absorption spectroscopy at FELs

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