Coupled electron–nuclear dynamics induced and monitored with femtosecond soft X-ray pulses in the amino acid glycine
Publication date
2024-02-05
Document type
Forschungsartikel
Author
Organisational unit
Publisher
American Chemical Society
Series or journal
The Journal of Physical Chemistry A
ISSN
Periodical volume
128
Periodical issue
6
First page
989
Last page
995
Peer-reviewed
✅
Part of the university bibliography
✅
Language
English
Keyword
Electrical energy
Molecules
Oscillation
Photoionization
Quantum mechanics
Abstract
The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures, and reaction mechanism of these many-body quantum objects are defined on the level of electrons and ions by molecular wave functions and their coherent superposition, respectively. In the present contribution, we monitor nonadiabatic quantum wave packet dynamics during molecular charge motion by reconstructing both the oscillatory charge density distribution and the characteristic time-dependent nuclear configuration coordinate from time-resolved Auger electron spectroscopic data recorded in previous studies on glycine molecules [Schwickert et al. Sci. Adv. 2022, 8, eabn6848]. The electronic and nuclear motion on the femtosecond time scale was induced and probed in kinematically complete soft X-ray experiments at the FLASH free-electron laser facility. The detailed analysis of amplitude, instantaneous phase, and instantaneous frequency of the propagating many-body wave packet during its lifecycle provides unprecedented insight into dynamical processes beyond the Born–Oppenheimer approximation. We are confident that the refined experimental data evaluation helps to develop new theoretical tools to describe time-dependent molecular wave functions in complicated but ubiquitous non-Born–Oppenheimer photochemical conditions.
Description
This article is licensed under a Creative Commons Attribution 4.0 International License (https://creativecommons.org/licenses/by/4.0/).
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Published version
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