Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS2Probed at the S 2p Edge
Year: 2023
Type: article
Abstract: High Resolution Image Download MS PowerPoint Slide Recent developments in X-ray free-electron lasers have enabled a novel site-selective probe of coupled nuclear and electronic dynamics in photoexcited molecules, time-resolved X-ray photoelectron spectroscopy (TRXPS). We present results from a joint experimental and theoretical TRXPS study of the well-characterized ultraviolet photodissociation of CS 2, a prototypical system for understanding non-adiabatic dynamics. These results demonstrate that the sulfur 2p binding energy is sensitive to changes in the nuclear structure following photoexcitation, which ultimately leads to dissociation into CS and S photoproducts. We are able to assign the main X-ray spectroscopic features to the CS and S products via comparison to a first-principles determination of the TRXPS based on ab initio multiple-spawning simulations. Our results demonstrate the use of TRXPS as a local probe of complex ultrafast photodissociation dynamics involving multimodal vibrational coupling, nonradiative transitions between electronic states, and multiple final product channels.
Authors: Ian Gabalski, Felix Allum, Issaka Seidu, Mathew Britton, Günter Brenner, Hubertus Bromberger, Mark Brouard, Philip H. Bucksbaum, Michael Burt, James P. Cryan, Taran Driver, Nagitha Ekanayake, Benjamin Erk, Diksha Garg, Eva Gougoula, David Heathcote, Paul Hockett, David M. P. Holland, Andrew J. Howard, Sonu Kumar, Jason W. L. Lee, Siqi Li, Joseph McManus, Jochen Mikosch, Dennis Milesevic, Russell S. Minns, Simon Neville, Atia-Tul-Noor, Christina C. Papadopoulou, Christopher Passow, Weronika O. Razmus, Anja Röder, Arnaud Rouzée, Alcides Simao, James Unwin, Claire Vallance, Tiffany Walmsley, Jun Wang, Daniel Rolles, Albert Stolow, Michael S. Schuurman, Ruaridh Forbes
Institutions: SLAC National Accelerator Laboratory, Stanford University, University of Oxford, Linac Coherent Light Source, National Research Council Canada, Deutsches Elektronen-Synchrotron DESY, Daresbury Laboratory, University of Kassel, University of Southampton, Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy, Kansas State University, University of Ottawa
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $5,000
Funders: National Science Foundation, U.S. Department of Defense, U.S. Department of Energy, University of Ottawa, UK Research and Innovation, CALIPSOplus, Leverhulme Trust, University of Southampton, European Commission, Helmholtz-Gemeinschaft, 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, Jesus College, University of Cambridge, Jesus College, University of Oxford, Deutsches Elektronen-Synchrotron, Horizon 2020, Division of Physics, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, H2020 European Research Council, H2020 Research Infrastructures, SLAC National Accelerator Laboratory
Awards: G1077140421, G1229526393, G1286251239, Convenient Access to Light Sources Open to Innovation, Science and to the World, G150693064, G1797787269, G2369733483, G2371548206, G2573442069, G262532246, G2673643517, Ultrafast Photochemical Dynamics in Complex Environments, G2978581158, G303061748, G304333627, G3145566345, G3474494657, G3530777102, G3643827549, 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, Convenient Access to Light Sources Open to Innovation, Science and to the World, G4654690619, G4758130757, 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, G585716984, Photoelectron interferometry as a structural and dynamical probe, G5996689310, G6033966476, G6550344761, G7214672632, 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, CAREER: Investigating Ultrafast Electronic and Structural Dynamics During Light-Driven Chemical Reactions, New Directions in Molecular Scattering: Multiple Pathways and Products, Time-Resolved Structural Imaging of Chemical Transition State Dynamics, G8382000481, Verbundprojekt 05K2016 - Nanoteilchenstruktur: Hochaufgelöste Struktur und Dynamik einzelner Nanoteilchen. Teilprojekt 1., G8726098666, G8945569637, G911061179, G969889393
OpenAlex ID: W4385514160