Journal Article

PUBDB-2025-03713

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Imaging a light-induced molecular elimination reaction with an X-ray free-electron laser

Li, X. (Corresponding author) ; Boll, R.XFEL.EU* ; Vindel-Zandbergen, P. ; González-Vázquez, J. ; Rivas, D.XFEL.EU* ; Bhattacharyya, S.Extern*XFEL.EU* ; Borne, K.Extern*XFEL.EU* ; Chen, K.Extern*XFEL.EU* ; De Fanis, A.XFEL.EU* ; Erk, B.XFEL.EU*DESY* ; Forbes, R.Extern*XFEL.EU* ; Green, A.Extern*XFEL.EU* ; Ilchen, M.XFEL.EU*DESY* ; Kaderiya, B.Extern* ; Kukk, E.Extern* ; Lam, H.Extern*XFEL.EU* ; Mazza, T.XFEL.EU* ; Mullins, T.XFEL.EU*DESY* ; Senfftleben, B.Extern*XFEL.EU*DESY* ; Trinter, F.Extern*XFEL.EU* ; Usenko, S.XFEL.EU* ; Venkatachalam, A.Extern*XFEL.EU* ; Wang, E.Extern* ; Cryan, J.Extern*XFEL.EU* ; Meyer, M.XFEL.EU* ; Jahnke, T.Extern*XFEL.EU*DESY* ; Ho, P.Extern*XFEL.EU* ; Rolles, D.Extern* ; Rudenko, A. (Corresponding author)Extern*

2025
Springer Nature [London]

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Please use a persistent id in citations: doi:10.1038/s41467-025-62274-z  doi:10.3204/PUBDB-2025-03713

Abstract: Tracking the motion of individual atoms during chemical reactions represents a severe experimental challenge, especially if several competing reaction pathways exist or if the reaction is governed by the correlated motion of more than two molecular constituents. Here we demonstrate how ultrashort X-ray pulses combined with coincident ion imaging can be used to trace molecular iodine elimination from laser-irradiated diiodomethane (CH2I2), a reaction channel of fundamental importance but small relative yield that involves the breaking of two molecular bonds and the formation of a new one. We map bending vibrations of the bound molecule, disentangle different dissociation pathways, image the correlated motion of the iodine atoms and the methylene group leading to molecular iodine ejection, and trace the vibrational motion of the formed product. Our results provide a quantitative mechanistic picture behind previously suggested reaction mechanisms and prove that a variety of geometries are involved in the molecular bond formation.

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Contributing Institute(s):

1. The European XFEL Users (XFEL-User)
2. SQS (XFEL_E2_SQS)
3. FLASH Photonen-Diagnose und Steuerungen (FS-FLASH-D)
4. FLASH Wissenschaftlicher Nutzerbetrieb (FS-FLASH-O)
5. Attosecond Science and Technology (FS-ATTO)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. DFG project G:(GEPRIS)509471550 - Dynamik photoionisations-induzierter Prozesse in laser-präparierten Molekülen in der Gasphase und der wässrigen Phase (509471550) (509471550)
3. AIM, DFG project G:(GEPRIS)390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)

Experiment(s):

1. SQS: Small Quantum Systems (SASE3)

Appears in the scientific report 2025

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