Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy

Mayer, D.; Gühr, M.; Squibb, R. J.; Calegari, F.; Wallner, M.; Düsterer, S.; Niebuhr, M.; Picconi, D.; Trabattoni, A.; Manschwetus, B.; Metje, J.; Wolf, T. J. A.; Ehlert, C.; Saalfrank, P.; Robinson, M. S.; Mazza, T.; Alisauskas, S.; Kuhlmann, M.; Lever, F.; Feifel, R.

doi:10.1038/s41467-021-27908-y

Journal Article

PUBDB-2022-00159

Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy

Mayer, D. ; Lever, F. ; Picconi, D. (Corresponding author) ; Metje, J. ; Alisauskas, S.DESY* ; Calegari, F.DESY* ; Düsterer, S.XFEL.EU*DESY* ; Ehlert, C.Extern* ; Feifel, R.Extern* ; Niebuhr, M. ; Manschwetus, B.DESY* ; Kuhlmann, M.DESY* ; Mazza, T.XFEL.EU* ; Robinson, M. S.CFEL*Extern*XFEL.EU* ; Squibb, R. J.Extern* ; Trabattoni, A.CFEL*DESY* ; Wallner, M.Extern* ; Saalfrank, P. ; Wolf, T. J. A.Extern*XFEL.EU* ; Gühr, M. (Corresponding author)Extern*XFEL.EU*

2022
Nature Publishing Group UK [London]

Nature Communications 13(1), 198 (2022) [10.1038/s41467-021-27908-y]

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Please use a persistent id in citations: doi:10.1038/s41467-021-27908-y doi:10.3204/PUBDB-2022-00159

Report No.: arXiv:2102.13431

Abstract: 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.

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ddc:500

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Experiment(s):

FLASH2 Beamline FL24 (FLASH2)

Appears in the scientific report 2022

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Medline

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