Journal Article

PUBDB-2022-03201

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy

Schwickert, D.Extern* ; Ruberti ; Kolorenc ; Przystawik, A.DESY* ; Skruszewicz, S.DESY* ; Sumfleth, M.Extern*DESY* ; Braune, M.XFEL.EU*DESY* ; Bocklage, L.XFEL.EU*DESY* ; Carretero Lopez, L.Extern*DESY* ; Czwalinna, M. K.DESY* ; Diaman, D.XFEL.EU*DESY* ; Duesterer, S.XFEL.EU*DESY* ; Kuhlmann, M.DESY* ; Palutke, S.CFEL*DESY* ; Roehlsberger, R.Extern*XFEL.EU*DESY* ; Rönsch-Schulenburg, J.DESY* ; Toleikis, S.XFEL.EU*DESY* ; Usenko, S.XFEL.EU* ; Viefhaus, J.Extern* ; Vorobiov ; Martins, M.Extern*XFEL.EU* ; Kip ; Averbukh, V.Extern* ; Marangos, J.Extern* ; Laarmann, T. (Corresponding author)XFEL.EU*DESY*

2022
AIP Publishing LLC Melville, NY

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Please use a persistent id in citations: doi:10.1063/4.0000165  doi:10.3204/PUBDB-2022-03201

Abstract: 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 $18.2 ^{+1.7}_{−1.4}≤𝑇≤23.9+1.2−1.1$ $fs.$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.

Note: Title is: Charge-induced chemical dynamics in glycine probed with time-resolved Auger electron spectroscopy

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)
2. FS-Photon Science (FS-PS)
3. FLASH Wissenschaftlicher Nutzerbetrieb (FS-FLASH-O)
4. FLASH Photonen-Diagnose und Steuerungen (FS-FLASH-D)
5. SQS (XFEL_E2_SQS)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. 6G2 - FLASH (DESY) (POF4-6G2) (POF4-6G2)
3. DFG project 390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)
4. DFG project 194651731 - EXC 1074: Hamburger Zentrum für ultraschnelle Beobachtung (CUI): Struktur, Dynamik und Kontrolle von Materie auf atomarer Skala (194651731) (194651731)
5. DFG project 170620586 - SFB 925: Licht-induzierte Dynamik und Kontrolle korrelierter Quantensysteme (170620586) (170620586)

Experiment(s):

1. FLASH2 Beamline FL24 (FLASH2)

Appears in the scientific report 2022

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