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Year of publication
Language
- English (43)
Is part of the Bibliography
- yes (43)
Keywords
- gamma rays: general (8)
- radiation mechanisms: non-thermal (8)
- gamma rays: galaxies (7)
- ISM: supernova remnants (6)
- galaxies: active (5)
- acceleration of particles (4)
- FLASH (3)
- ISM: clouds (3)
- cosmic rays (3)
- Auger–Meitner (2)
Institute
Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
(2022)
Mayer, Dennis ; Lever, Fabiano ; Picconi, David ; Metje, Jan ; Ališauskas, Skirmantas ; Calegari, Francesca ; Düsterer, Stefan ; Ehlert, Christopher ; Feifel, Raimund ; Niebuhr, Mario ; Manschwetus, Bastian ; Kuhlmann, Marion ; Mazza, Tommaso ; Robinson, Matthew Scott ; Squibb, Richard James ; Trabattoni, Andrea ; Wallner, Måns ; Saalfrank, Peter ; Wolf, Thomas J. A. ; Gühr, Markus
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.
Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
(2022)
Mayer, Dennis ; Lever, Fabiano ; Picconi, David ; Metje, Jan ; Ališauskas, Skirmantas ; Calegari, Francesca ; Düsterer, Stefan ; Ehlert, Christopher ; Feifel, Raimund ; Niebuhr, Mario ; Manschwetus, Bastian ; Kuhlmann, Marion ; Mazza, Tommaso ; Robinson, Matthew Scott ; Squibb, Richard James ; Trabattoni, Andrea ; Wallner, Måns ; Saalfrank, Peter ; Wolf, Thomas J. A. ; Gühr, Markus
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.
Lever, Fabiano ; Mayer, Dennis ; Metje, Jan ; Alisauskas, Skirmantas ; Calegari, Francesca ; Düsterer, Stefan ; Feifel, Raimund ; Niebuhr, Mario ; Manschwetus, Bastian ; Kuhlmann, Marion ; Mazza, Tommaso ; Robinson, Matthew Scott ; Squibb, Richard J. ; Trabattoni, Andrea ; Wallner, Måns ; Wolf, Thomas J. A. ; Gühr, Markus
In this paper, we report X-ray absorption and core-level electron spectra of the nucleobase derivative 2-thiouracil at the sulfur L1- and L2,3-edges. We used soft X-rays from the free-electron laser FLASH2 for the excitation of isolated molecules and dispersed the outgoing electrons with a magnetic bottle spectrometer. We identified photoelectrons from the 2p core orbital, accompanied by an electron correlation satellite, as well as resonant and non-resonant Coster–Kronig and Auger–Meitner emission at the L1- and L2,3-edges, respectively. We used the electron yield to construct X-ray absorption spectra at the two edges. The experimental data obtained are put in the context of the literature currently available on sulfur core-level and 2-thiouracil spectroscopy.