Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses
Abstract 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 p...
Guardado en:
| Autores principales: | , , , , , , , , , , , , , , , , , , , |
|---|---|
| Formato: | article |
| Lenguaje: | EN |
| Publicado: |
Nature Portfolio
2021
|
| Materias: | |
| Acceso en línea: | https://doaj.org/article/18c7f31e73ec4f57a2cc149d32a0abb6 |
| Etiquetas: |
Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
|
| id |
oai:doaj.org-article:18c7f31e73ec4f57a2cc149d32a0abb6 |
|---|---|
| record_format |
dspace |
| spelling |
oai:doaj.org-article:18c7f31e73ec4f57a2cc149d32a0abb62021-12-02T14:12:42ZElectron-ion coincidence measurements of molecular dynamics with intense X-ray pulses10.1038/s41598-020-79818-62045-2322https://doaj.org/article/18c7f31e73ec4f57a2cc149d32a0abb62021-01-01T00:00:00Zhttps://doi.org/10.1038/s41598-020-79818-6https://doaj.org/toc/2045-2322Abstract 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 N $$_2$$ 2 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.Xiang LiLudger InhesterTimur OsipovRebecca BollRyan CoffeeJames CryanAve GattonTais GorkhoverGregor HartmanMarkus IlchenAndré KnieMing-Fu LinMichael P. MinittiClemens WeningerThomas J. A. WolfSang-Kil SonRobin SantraDaniel RollesArtem RudenkoPeter WalterNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 11, Iss 1, Pp 1-12 (2021) |
| institution |
DOAJ |
| collection |
DOAJ |
| language |
EN |
| topic |
Medicine R Science Q |
| spellingShingle |
Medicine R Science Q Xiang Li Ludger Inhester Timur Osipov Rebecca Boll Ryan Coffee James Cryan Ave Gatton Tais Gorkhover Gregor Hartman Markus Ilchen André Knie Ming-Fu Lin Michael P. Minitti Clemens Weninger Thomas J. A. Wolf Sang-Kil Son Robin Santra Daniel Rolles Artem Rudenko Peter Walter Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses |
| description |
Abstract 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 N $$_2$$ 2 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. |
| format |
article |
| author |
Xiang Li Ludger Inhester Timur Osipov Rebecca Boll Ryan Coffee James Cryan Ave Gatton Tais Gorkhover Gregor Hartman Markus Ilchen André Knie Ming-Fu Lin Michael P. Minitti Clemens Weninger Thomas J. A. Wolf Sang-Kil Son Robin Santra Daniel Rolles Artem Rudenko Peter Walter |
| author_facet |
Xiang Li Ludger Inhester Timur Osipov Rebecca Boll Ryan Coffee James Cryan Ave Gatton Tais Gorkhover Gregor Hartman Markus Ilchen André Knie Ming-Fu Lin Michael P. Minitti Clemens Weninger Thomas J. A. Wolf Sang-Kil Son Robin Santra Daniel Rolles Artem Rudenko Peter Walter |
| author_sort |
Xiang Li |
| title |
Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses |
| title_short |
Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses |
| title_full |
Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses |
| title_fullStr |
Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses |
| title_full_unstemmed |
Electron-ion coincidence measurements of molecular dynamics with intense X-ray pulses |
| title_sort |
electron-ion coincidence measurements of molecular dynamics with intense x-ray pulses |
| publisher |
Nature Portfolio |
| publishDate |
2021 |
| url |
https://doaj.org/article/18c7f31e73ec4f57a2cc149d32a0abb6 |
| work_keys_str_mv |
AT xiangli electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT ludgerinhester electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT timurosipov electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT rebeccaboll electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT ryancoffee electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT jamescryan electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT avegatton electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT taisgorkhover electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT gregorhartman electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT markusilchen electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT andreknie electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT mingfulin electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT michaelpminitti electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT clemensweninger electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT thomasjawolf electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT sangkilson electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT robinsantra electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT danielrolles electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT artemrudenko electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses AT peterwalter electronioncoincidencemeasurementsofmoleculardynamicswithintensexraypulses |
| _version_ |
1718391771803680768 |