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Imaging a light-induced molecular elimination reaction with an X-ray free-electron laser

Xiang Li (), Rebecca Boll, Patricia Vindel-Zandbergen, Jesús González-Vázquez, Daniel E. Rivas, Surjendu Bhattacharyya, Kurtis Borne, Keyu Chen, Alberto Fanis, Benjamin Erk, Ruaridh Forbes, Alice E. Green, Markus Ilchen, Balram Kaderiya, Edwin Kukk, Huynh Van Sa Lam, Tommaso Mazza, Terence Mullins, Björn Senfftleben, Florian Trinter, Sergey Usenko, Anbu Selvam Venkatachalam, Enliang Wang, James P. Cryan, Michael Meyer, Till Jahnke, Phay J. Ho, Daniel Rolles and Artem Rudenko ()
Additional contact information
Xiang Li: Linac Coherent Light Source, SLAC National Accelerator Laboratory
Rebecca Boll: Holzkoppel 4
Patricia Vindel-Zandbergen: Department of Chemistry, New York University
Jesús González-Vázquez: Cantoblanco
Daniel E. Rivas: Holzkoppel 4
Surjendu Bhattacharyya: Kansas State University
Kurtis Borne: Kansas State University
Keyu Chen: Kansas State University
Alberto Fanis: Holzkoppel 4
Benjamin Erk: Notkestrasse 85
Ruaridh Forbes: Linac Coherent Light Source, SLAC National Accelerator Laboratory
Alice E. Green: Holzkoppel 4
Markus Ilchen: Holzkoppel 4
Balram Kaderiya: Kansas State University
Edwin Kukk: Department of Physics and Astronomy, University of Turku
Huynh Van Sa Lam: Kansas State University
Tommaso Mazza: Holzkoppel 4
Terence Mullins: Holzkoppel 4
Björn Senfftleben: Holzkoppel 4
Florian Trinter: Molecular Physics, Fritz-Haber-Institut der Max-Planck-Gesellschaft
Sergey Usenko: Holzkoppel 4
Anbu Selvam Venkatachalam: Kansas State University
Enliang Wang: Kansas State University
James P. Cryan: Linac Coherent Light Source, SLAC National Accelerator Laboratory
Michael Meyer: Holzkoppel 4
Till Jahnke: Holzkoppel 4
Phay J. Ho: Argonne National Laboratory
Daniel Rolles: Kansas State University
Artem Rudenko: Kansas State University

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-62274-z

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