Year: 2024
Type: preprint
Abstract: We present an investigation of the ultrafast dynamics of the polycyclic aromatic hydrocarbon fluorene initiated by an intense femtosecond near- infrared laser pulse (810 nm) and probed by a weak visible pulse (405 nm). Using a multichannel detection scheme (mass spectra, electron and ion velocity-map imaging), we provide a full disentanglement of the complex dynamics of the vibronically excited parent molecule, its excited ionic states, and fragments. We observed various channels resulting from the strong-field ionization regime. In particular, we observed the formation of the unstable tetracation of fluorene, above-threshold ionization features in the photoelectron spectra, and evidence of ubiquitous secondary fragmentation. We produced a global fit of all observed time-dependent photoelectron and photoion channels. This global fit includes four parent ions extracted from the mass spectra, 15 kinetic-energy-resolved ionic fragments extracted from ion velocity map imaging, and five photoelectron channels obtained from electron velocity map imaging. The fit allowed for the extraction of 60 lifetimes of various metastable photoinduced intermediates.
Source: ChemRxiv
Authors: Diksha Garg, Pragya Chopra, Jason W. L. Lee, Denis Tikhonov, Sonu Kumar, Oender Akcaalan, Felix Allum, Rebecca Boll, Alexander A. Butler, Benjamin Erk, Eva Gougoula, Sébastien P. Gruet, Lanhai He, David Heathcote, Ellen Jones, Mehdi M. Kazemi, Jan Lahl, Alexander K. Lemmens, Zhihao Liu, Donatella Loru, Sylvain Maclot, Robert Mason, James Merrick, Erland Müller, Terry Mullins, Christina C. Papadopoulou, Christopher Passow, Jasper Peschel, Marius Plach, Daniel Ramm, Patrick Robertson, Dimitrios Rompotis, Alcides Simao, Amanda L. Steber, Ayhan Tajalli, Atia Tul-Noor, Nidin Vadassery, Ivo S. Vinklarek, Simone Techert, Jochen Küpper, Anouk M. Rijs, Daniel Rolles, Mark Brouard, Sadia Bari, Per Eng-Johnsson, Claire Vallance, Michael Burt, Bastian Manschwetus, Melanie Schnell
Institutions: Universität Hamburg, Deutsches Elektronen-Synchrotron DESY, University of Oxford, SLAC National Accelerator Laboratory, European X-Ray Free-Electron Laser, Lund University, HFML-FELIX, University of Amsterdam, Lyon 1 Université, Ruhr University Bochum, Universidad de Valladolid, Vrije Universiteit Amsterdam, Kansas State University, University of Groningen, Photonics (United States), Christian-Albrechts-Universität zu Kiel
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
Funders: National Science Foundation, CALIPSOplus, University College, Oxford, Deutsche Forschungsgemeinschaft, Bundesministerium für Bildung und Forschung, Knut och Alice Wallenbergs Stiftelse, Max-Planck-Gesellschaft, Vetenskapsrådet, Engineering and Physical Sciences Research Council, Deutsches Elektronen-Synchrotron, Horizon 2020
Awards: G1077140421, G1230266125, G1434330249, G1797787269, G1981296498, G2573442069, Ultrafast Photochemical Dynamics in Complex Environments, G2978581158, G304333627, EXC 2056: CUI: Advanced Imaging of Matter, G3530777102, G4336652674, 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'., Verbundprojekt FSP 302 - Freie-Elektronen-Laser: Nanoskopische Systeme. Teilprojekt 4: Dynamik einzelner Nanoteilchen in Femtosekunden-Zeitlupe - Filmen mit ultrakurzen Röntgen-Doppelpulsen., G516729603, Imaging Chemical Dynamics with Ultrafast Laser Spectroscopy, G5486038727, G5631081224, G585716984, G6033966476, 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'., CAREER: Investigating Ultrafast Electronic and Structural Dynamics During Light-Driven Chemical Reactions, New Directions in Molecular Scattering: Multiple Pathways and Products, G8433356701, Verbundprojekt 05K2016 - Nanoteilchenstruktur: Hochaufgelöste Struktur und Dynamik einzelner Nanoteilchen. Teilprojekt 1.
OpenAlex ID: W4391746278