Year: 2024
Type: article
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.
DOI: 10.1039/d3cp05063g
Authors: Diksha Garg, Pragya Chopra, Jason W. L. Lee, Denis S. 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. Vinklárek, 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, Christian-Albrechts-Universität zu Kiel, University of Oxford, European X-Ray Free-Electron Laser, Center for Free-Electron Laser Science, Lund University, Radboud University Nijmegen, HFML-FELIX, University of Amsterdam, Lyon 1 Université, Hamburg Centre for Ultrafast Imaging, Vrije Universiteit Amsterdam, Kansas State University, University of Groningen, Zernike Institute for Advanced Materials
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: bronze
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, European Research Council, Deutsches Elektronen-Synchrotron, Horizon 2020, H2020 European Research Council
Awards: G1077140421, G1230266125, G1434330249, EXC 2033: RESOLV (Ruhr Explores Solvation), G1797787269, G1981296498, G2573442069, Ultrafast Photochemical Dynamics in Complex Environments, G274347230, 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, 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, Attosecond electron-nuclear dynamics studied using intense XUV and X-ray laser pulses, G8433356701, Verbundprojekt 05K2016 - Nanoteilchenstruktur: Hochaufgelöste Struktur und Dynamik einzelner Nanoteilchen. Teilprojekt 1., G988628021
OpenAlex ID: W4399856804