Coupled electron-nuclear dynamics induced and monitored with femtosecond soft X-ray pulses in the amino acid glycine
Author(s)
Type
Journal Article
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.
Date Issued
2024-02-15
Date Acceptance
2024-01-15
Citation
The Journal of Physical Chemistry A: Isolated Molecules, Clusters, Radicals, and Ions; Environmental Chemistry, Geochemistry, and Astrochemistry; Theory, 2024, 128 (6), pp.989-995
ISSN
1089-5639
Publisher
American Chemical Society
Start Page
989
End Page
995
Journal / Book Title
The Journal of Physical Chemistry A: Isolated Molecules, Clusters, Radicals, and Ions; Environmental Chemistry, Geochemistry, and Astrochemistry; Theory
Volume
128
Issue
6
Copyright Statement
Copyright © 2024 The Authors. Published by American Chemical Society. This publication is licensed under
CC-BY 4.0.
CC-BY 4.0.
License URL
Identifier
https://www.ncbi.nlm.nih.gov/pubmed/38315166
Publication Status
Published
Coverage Spatial
United States
Date Publish Online
2024-02-05