Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses
Autor: | Gregor Hartman, Markus Ilchen, James P. Cryan, Clemens Weninger, Ryan Coffee, Daniel Rolles, Sang-Kil Son, Robin Santra, Rebecca Boll, Ludger Inhester, Ave Gatton, André Knie, Artem Rudenko, Tais Gorkhover, Peter Walter, Ming-Fu Lin, Michael P. Minitti, Thomas J. A. Wolf, Xiang Li, Timur Osipov |
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Jazyk: | angličtina |
Rok vydání: | 2021 |
Předmět: |
Photon
Photoemission spectroscopy Science Ionic bonding 02 engineering and technology Electron 01 natural sciences Article Ion X-rays 0103 physical sciences Physics::Atomic and Molecular Clusters 010306 general physics Absorption (electromagnetic radiation) Physics Multidisciplinary Atomic and molecular interactions with photons Photoelectric effect 021001 nanoscience & nanotechnology Dication Medicine Atomic physics 0210 nano-technology ddc:600 |
Zdroj: | Scientific Reports, Vol 11, Iss 1, Pp 1-12 (2021) Scientific reports 11(1), 505 (2021). doi:10.1038/s41598-020-79818-6 Scientific Reports |
ISSN: | 2045-2322 |
Popis: | Scientific reports 11(1), 505 (2021). doi:10.1038/s41598-020-79818-6 Molecules can sequentially absorb multiple photons when irradiated by an intense X-ray pulse from a free-electron laser. If the time delay between two photoabsorption events can be determined, this enables pump-probe experiments with a single X-ray pulse, where the absorption of the first photon induces electronic and nuclear dynamics that are probed by the absorption of the second photon. Here we show a realization of such a single-pulse X-ray pump-probe scheme on N2 molecules, using the X-ray induced dissociation process as an internal clock that is read out via coincident detection of photoelectrons and fragment ions. By coincidence analysis of the kinetic energies of the ionic fragments and photoelectrons, the transition from a bound molecular dication to two isolated atomic ions is observed through the energy shift of the inner-shell electrons. Via ab-initio simulations, we are able to map characteristic features in the kinetic energy release and photoelectron spectrum to specific delay times between photoabsorptions. In contrast to previous studies where nuclear motions were typically revealed by measuring ion kinetics, our work shows that inner-shell photoelectron energies can also be sensitive probes of nuclear dynamics, which adds one more dimension to the study of light-matter interactions with X-ray pulses. Published by Macmillan Publishers Limited, part of Springer Nature, [London] |
Databáze: | OpenAIRE |
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