TY  - GEN
A1  - Mayer, Dennis
A1  - Lever, Fabiano
A1  - Picconi, David
A1  - Metje, Jan
A1  - Ališauskas, Skirmantas
A1  - Calegari, Francesca
A1  - Düsterer, Stefan
A1  - Ehlert, Christopher
A1  - Feifel, Raimund
A1  - Niebuhr, Mario
A1  - Manschwetus, Bastian
A1  - Kuhlmann, Marion
A1  - Mazza, Tommaso
A1  - Robinson, Matthew Scott
A1  - Squibb, Richard James
A1  - Trabattoni, Andrea
A1  - Wallner, Måns
A1  - Saalfrank, Peter
A1  - Wolf, Thomas J. A.
A1  - Gühr, Markus
T1  - Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
T2  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe
N2  - The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220–250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1301 
Y1  - 2022
UR  - https://publishup.uni-potsdam.de/frontdoor/index/index/docId/57744
UR  - https://nbn-resolving.org/urn:nbn:de:kobv:517-opus4-577442
SN  - 1866-8372
N1  - These authors contributed equally: D. Mayer, F. Lever.

A Publisher Correction to this article was published on 09 March 2022.

This article has been updated.
IS  - 1301
ER  -