| Autor: |
David Schwickert, Marco Ruberti, Přemysl Kolorenč, Andreas Przystawik, Slawomir Skruszewicz, Malte Sumfleth, Markus Braune, Lars Bocklage, Luis Carretero, Marie Kristin Czwalinna, Dian Diaman, Stefan Düsterer, Marion Kuhlmann, Steffen Palutke, Ralf Röhlsberger, Juliane Rönsch-Schulenburg, Sven Toleikis, Sergey Usenko, Jens Viefhaus, Anton Vorobiov, Michael Martins, Detlef Kip, Vitali Averbukh, Jon P. Marangos, Tim Laarmann |
| Jazyk: |
angličtina |
| Rok vydání: |
2022 |
| Předmět: |
|
| Zdroj: |
Structural Dynamics, Vol 9, Iss 6, Pp 064301-064301-12 (2022) |
| Druh dokumentu: |
article |
| ISSN: |
2329-7778 |
| DOI: |
10.1063/4.0000165 |
| Popis: |
In the present contribution, we use x-rays to monitor charge-induced chemical dynamics in the photoionized amino acid glycine with femtosecond time resolution. The outgoing photoelectron leaves behind the cation in a coherent superposition of quantum mechanical eigenstates. Delayed x-ray pulses track the induced coherence through resonant x-ray absorption that induces Auger decay. Temporal modulation of the Auger electron signal correlated with specific ions is observed, which is governed by the initial electronic coherence and subsequent vibronic coupling to nuclear degrees of freedom. In the time-resolved x-ray absorption measurement, we monitor the time-frequency spectra of the resulting many-body quantum wave packets for a period of 175 fs along different reaction coordinates. Our experiment proves that by measuring specific fragments associated with the glycine dication as a function of the pump-probe delay, one can selectively probe electronic coherences at early times associated with a few distinguishable components of the broad electronic wave packet created initially by the pump pulse in the cation. The corresponding coherent superpositions formed by subsets of electronic eigenstates and evolving along parallel dynamical pathways show different phases and time periods in the range of ( − 0.3 ± 0.1 ) π ≤ ϕ ≤ ( 0.1 ± 0.2 ) π and 18.2 − 1.4 + 1.7 ≤ T ≤ 23.9 − 1.1 + 1.2 fs. Furthermore, for long delays, the data allow us to pinpoint the driving vibrational modes of chemical dynamics mediating charge-induced bond cleavage along different reaction coordinates. |
| Databáze: |
Directory of Open Access Journals |
| Externí odkaz: |
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