X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2
Year: 2023
Type: article
Abstract: Structural imaging of transient excited-state species is a key goal of molecular physics, promising to unveil rich information about the dynamics underpinning photochemical transformations. However, separating the electronic and nuclear contributions to the spectroscopic observables is challenging, and typically requires the application of high-level theory. Here, we employ site-selective ionisation via ultrashort soft X-ray pulses and time-resolved Coulomb explosion imaging to interrogate structural dynamics of the ultraviolet photochemistry of carbon disulfide. This prototypical system exhibits the complex motifs of polyatomic photochemistry, including strong non-adiabatic couplings, vibrational mode couplings, and intersystem crossing. Immediately following photoexcitation, we observe Coulomb explosion signatures of highly bent and stretched excited-state geometries involved in the photodissociation. Aided by a model to interpret such changes, we build a comprehensive picture of the photoinduced nuclear dynamics that follows initial bending and stretching motions, as the reaction proceeds towards photodissociation.
Source: Communications Physics
Authors: James Unwin, Felix Allum, Mathew Britton, Ian Gabalski, Hubertus Bromberger, Mark Brouard, Philip H. Bucksbaum, Taran Driver, Nagitha Ekanayake, Diksha Garg, Eva Gougoula, David Heathcote, Andrew J. Howard, Paul Hockett, David M. P. Holland, Sonu Kumar, Chow-shing Lam, Jason W. L. Lee, Joseph McManus, Jochen Mikosch, Dennis Milesevic, Russell S. Minns, Christina C. Papadopoulou, Christopher Passow, Weronika O. Razmus, Anja Röder, Arnaud Rouzée, Michael Schuurman, Alcides Simao, Albert Stolow, Atia Tul-Noor, Claire Vallance, Tiffany Walmsley, Daniel Rolles, Benjamin Erk, Michael Burt, Ruaridh Forbes
Institutions: University of Oxford, SLAC National Accelerator Laboratory, Linac Coherent Light Source, Stanford University, Deutsches Elektronen-Synchrotron DESY, National Research Council Canada, Daresbury Laboratory, Universität Hamburg, University of Kassel, University of Southampton, Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy, University of Ottawa, Ruhr University Bochum, Kansas State University
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $3,690
Funders: U.S. Department of Energy, University of Ottawa, UK Research and Innovation, CALIPSOplus, Leverhulme Trust, University of Southampton, European Commission, Bundesministerium für Bildung und Forschung, Max-Planck-Gesellschaft, Office of Science, National Defense Science and Engineering Graduate, Natural Sciences and Engineering Research Council of Canada, Engineering and Physical Sciences Research Council, Science and Technology Facilities Council, Deutsches Elektronen-Synchrotron, Horizon 2020, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, SLAC National Accelerator Laboratory
Awards: G1077140421, G1229526393, G1286251239, Convenient Access to Light Sources Open to Innovation, Science and to the World, G1797787269, G1815137805, G222768804, G2371548206, G2573442069, G262532246, Ultrafast Photochemical Dynamics in Complex Environments, STRUCTURE AND DYNAMICS OF ATOMS, IONS, MOLECULES AND SURFACES, G2975900969, G2978581158, G303061748, G333714909, G3474494657, G3530777102, G3826261775, G4235786860, G4336652674, G434337789, Verbundprojekt: FSP 301 - FLASH: Nanoskopische Systeme. Teilprojekt 1.1: Universelle Experimentierkammer für Streuexperimente mit kohärenten Femtosekunden-Röntgenpulsen Multi Purpose Coherent Scattering Chamber for FLASH and XFEL 'MPscatt'., G457067979, G4673714799, Verbundprojekt FSP 302 - Freie-Elektronen-Laser: Nanoskopische Systeme. Teilprojekt 4: Dynamik einzelner Nanoteilchen in Femtosekunden-Zeitlupe - Filmen mit ultrakurzen Röntgen-Doppelpulsen., G495301720, G498139845, G5085731485, G516729603, G5368910837, Imaging Chemical Dynamics with Ultrafast Laser Spectroscopy, G5486038727, G5570207115, G5648016710, G585716984, G5996689310, G6033966476, G6550344761, G6824076759, ATOMIC PHYSICS WITH HIGHLY CHARGED IONS, G7283024673, G7331630580, Verbundprojekt: FSP 301 - FLASH: Nanoskopische Systeme. Teilprojekt 1.2: Universelle Experimentierkammer für Streuexperimente mit kohärenten Femtosekunden-Röntgenpulsen Multi Purpose Coherent Scattering Chamber for FLASH and XFEL 'MPscatt'., G753646987, G8382000481, Verbundprojekt 05K2016 - Nanoteilchenstruktur: Hochaufgelöste Struktur und Dynamik einzelner Nanoteilchen. Teilprojekt 1., G8726098666, G8945569637, G911061179, G969889393, STRUCTURE AND DYNAMICS OF ATOMS, IONS, MOLECULES AND SURFACES
OpenAlex ID: W4387811564