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Abstract
We present the results of a combined experimental and numerical study on strong-field ionisation of acetylene performed with the aim of identifying the mechanism behind the previously reported surprisingly large multi-electron ionisation probabilities of polyatomic molecules. Using coincidence momentum imaging techniques and time-dependent density functional simulations, we show that the reported efficient ionisation is due to the combined action of a significant geometrically induced energy upshift of the most relevant valence orbitals as the C-H distance stretches beyond about two times the equilibrium distance, and a strong increase in the coupling between multiple molecular orbitals concomitant with this stretch motion. The identified enhanced ionisation mechanism, which we refer to as EIC-MOUSE, is only effective for molecules aligned close to parallel to the laser polarisation direction, and is inhibited for perpendicularly aligned molecules because of a suppression of the C-H stretch motion during the onset of ionisation.
Originalsprache | englisch |
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Aufsatznummer | 125601 |
Seitenumfang | 18 |
Fachzeitschrift | Journal of Physics B: Atomic, Molecular and Optical Physics |
Jahrgang | 50 |
Ausgabenummer | 12 |
DOIs | |
Publikationsstatus | Veröffentlicht - 31 Mai 2017 |
ASJC Scopus subject areas
- Atom- und Molekularphysik sowie Optik
- Physik der kondensierten Materie
Fields of Expertise
- Advanced Materials Science
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FWF - Photoinduzierte Dynamiken - Photoinduzierte Dynamiken in einer Quantenflüssigkeit
1/09/16 → 31/08/20
Projekt: Forschungsprojekt