Erlangen 2022 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 2: X-ray FELs (joint session MO/A)
MO 2.1: Vortrag
Montag, 14. März 2022, 14:00–14:15, MO-H5
Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy — •Dennis Mayer1, Fabiano Lever1, David Picconi1, Jan Metje1, Skirmantas Alisauskas2, Francesca Calegari3, Stefan Düsterer2, Christopher Ehlert4, Raimund Feiffel5, Mario Niebuhr1, Bastian Manschwetus2, Marion Kuhlmann2, Tomaso Mazza6, Matthew S. Robinson1,3, Richard J. Squibb5, Andrea Trabattoni3, Mans Wallner5, Peter Saalfrank1, Thomas J.A. Wolf7, and Markus Gühr1 — 1University of Potsdam, Germany — 2DESY, Hamburg, Germany — 3CFEL, Hamburg, Germany — 4HITS gGmbH, Heidelberg, Germany — 5University of Gothenburg, Sweden — 6European XFEL GmbH, Hamburg, Germany — 7Stanford PULSE Institute, Menlo Park, USA
We demonstrate the capabilities of time-resolved x-ray photoelectron spectroscopy with a study of the UV-excited dynamics of 2-thiouracil conducted at the FLASH free electron laser in Hamburg, Germany. By probing sulfur 2p core electrons, we discover that a significant part of the excited-state population relaxes to the ground state within 220-250fs. Observed spectral shifts can be directly attributed to a charge redistribution over the molecule during the relaxation process. Additionally, we observe a 250fs oscillation in the kinetic energy of the excited-state population which reveals a coherent population exchange among electronic states.