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

Li, Xiang; Boll, Rebecca; Vindel-Zandbergen, Patricia; González-Vázquez, Jesús; Rivas, Daniel E.; Bhattacharyya, Surjendu; Borne, Kurtis; Chen, Keyu; De Fanis, Alberto; Erk, Benjamin; Forbes, Ruaridh; Green, Alice E.; Ilchen, Markus; Kaderiya, Balram; Kukk, Edwin; Lam, Huynh Van Sa; Mazza, Tommaso; Mullins, Terence; Senfftleben, Björn; Trinter, Florian; Usenko, Sergey; Venkatachalam, Anbu Selvam; Wang, Enliang; Cryan, James P.; Meyer, Michael; Jahnke, Till; Ho, Phay J.; Rolles, Daniel; Rudenko, Artem

doi:10.1038/s41467-025-62274-z

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

Journal Article · Wed Jul 30 00:00:00 UTC 2025 · Nature Communications

DOI: https://doi.org/10.1038/s41467-025-62274-z · OSTI ID:3003077

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SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
European XFEL, Schenefeld (Germany)
New York University, NY (United States)
Universidad Autónoma de Madrid (Spain)
Kansas State University, Manhattan, KS (United States)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); University of California, Davis, CA (United States)
European XFEL, Schenefeld (Germany); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); University of Edinburgh (United Kingdom)
European XFEL, Schenefeld (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); University of Hamburg (Germany)
University of Turku (Finland)
European XFEL, Schenefeld (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Universität Hamburg (Germany)
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Berlin (Germany); Goethe-Universität Frankfurt (Germany)
European XFEL, Schenefeld (Germany); Max-Planck-Institut für Kernphysik, Heidelberg (Germany)
Argonne National Laboratory (ANL), Argonne, IL (United States)

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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Research Organization:: Kansas State University, Manhattan, KS (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Bundesministerium für Bildung und Forschung (BMBF); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; FG02-86ER13491; SC0020276

OSTI ID:: 3003077

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 16; ISSN 2041-1723

Publisher:: Springer Science and Business Media LLCCopyright Statement

Country of Publication:: United States

Language:: English

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