Fragmentation Dynamics of Fluorene Explored Using Ultrafast XUV-Vis Pump-Probe Spectroscopy

D. Garg, J. W.L. Lee, D. S. Tikhonov, P. Chopra, A. L. Steber, A. K. Lemmens, B. Erk, F. Allum, R. Boll, X. Cheng, S. Düsterer, S. Gruet, L. He, D. Heathcote, M. Johny, M. M. Kazemi, H. Köckert, J. Lahl, D. Loru, S. MaclotR. Mason, E. Müller, T. Mullins, P. Olshin, C. Passow, J. Peschel, D. Ramm, D. Rompotis, S. Trippel, J. Wiese, F. Ziaee, S. Bari, M. Burt, J. Küpper, A. M. Rijs, D. Rolles, S. Techert, P. Eng-Johnsson, M. Brouard, C. Vallance, B. Manschwetus, M. Schnell*

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

We report on the use of extreme ultraviolet (XUV, 30.3 nm) radiation from the Free-electron LASer in Hamburg (FLASH) and visible (Vis, 405 nm) photons from an optical laser to investigate the relaxation and fragmentation dynamics of fluorene ions. The ultrashort laser pulses allow to resolve the molecular processes occurring on the femtosecond timescales. Fluorene is a prototypical small polycyclic aromatic hydrocarbon (PAH). Through their infrared emission signature, PAHs have been shown to be ubiquitous in the universe, and they are assumed to play an important role in the chemistry of the interstellar medium. Our experiments track the ionization and dissociative ionization products of fluorene through time-of-flight mass spectrometry and velocity-map imaging. Multiple processes involved in the formation of each of the fragment ions are disentangled through analysis of the ion images. The relaxation lifetimes of the excited fluorene monocation and dication obtained through the fragment formation channels are reported to be in the range of a few tens of femtoseconds to a few picoseconds.

Original languageEnglish
Article number880793
Pages (from-to)1-12
Number of pages12
JournalFrontiers in Physics
Volume10
Issue numberMay
Early online date12 May 2022
DOIs
Publication statusPublished - May 2022

Bibliographical note

Funding Information:
This work was supported by the ERC Starting Grant ASTROROT, grant number 638027, and the project CALIPSOplus under the grant agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. The experimental parts of this research were carried out at beamline BL1 FLASH at DESY, a member of the Helmholtz Association (HGF). Beamtime was allocated for proposal F-20170540. We acknowledge the Max Planck Society for funding the development and the initial operation of the CAMP end-station within the Max Planck Advanced Study Group at CFEL and for providing this equipment for CAMP@FLASH. The installation of CAMP@FLASH was partially funded by the BMBF grants 05K10KT2, 05K13KT2, 05K16KT3, and 05K10KTB from FSP-302. We acknowledge financial support by the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement 641789 “Molecular Electron Dynamics investigated by Intense Fields and Attosecond Pulses” (MEDEA), the Clusters of Excellence “Center for Ultrafast Imaging” (CUI, EXC 1074, ID 194651731), the “Advanced Imaging of Matter” (AIM, EXC 2056, ID 390715994) of the Deutsche Forschungsgemeinschaft (DFG), the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007–2013) through the Consolidator Grant COMOTION (614507), and the Helmholtz Gemeinschaft through the “Impuls- und Vernetzungsfonds”. In addition, the project was supported by The Netherlands Organization for Scientific Research (NWO) and is part of the Dutch Astrochemistry Network (DAN) II (Project No. 648.000.029). PE-J, SM, and JP acknowledge support from the Swedish Research Council and the Swedish Foundation for Strategic Research. The authors are additionally thankful for the support from the following funding bodies: the UK EPSRC (MBR and CV-EP/L005913/1 and EP/V026690/1; MBU-EP/S028617/1), STFC (PNPAS award and mini-IPS Grant No. ST/J002895/1), the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy (FZ—DE-FG02-86ER13491); the National Science Foundation (DR - PHYS-1753324); and the Helmholtz Initiative and Networking Fund through the Young Investigators Group Program (SB). We acknowledge the use of the Maxwell computational resources operated at Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany.

Funding Information:
This work was supported by the ERC Starting Grant ASTROROT, grant number 638027, and the project CALIPSOplus under the grant agreement 730872 from the EU Framework Programme for Research and Innovation HORIZON 2020. The experimental parts of this research were carried out at beamline BL1 FLASH at DESY, a member of the Helmholtz Association (HGF). Beamtime was allocated for proposal F-20170540. We acknowledge the Max Planck Society for funding the development and the initial operation of the CAMP end-station within the Max Planck Advanced Study Group at CFEL and for providing this equipment for CAMP@FLASH. The installation of CAMP@FLASH was partially funded by the BMBF grants 05K10KT2, 05K13KT2, 05K16KT3, and 05K10KTB from FSP-302. We acknowledge financial support by the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement 641789 “Molecular Electron Dynamics investigated by Intense Fields and Attosecond Pulses” (MEDEA), the Clusters of Excellence “Center for Ultrafast Imaging” (CUI, EXC 1074, ID 194651731), the “Advanced Imaging of Matter” (AIM, EXC 2056, ID 390715994) of the Deutsche Forschungsgemeinschaft (DFG), the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007–2013) through the Consolidator Grant COMOTION (614507), and the Helmholtz Gemeinschaft through the “Impuls- und Vernetzungsfonds”. In addition, the project was supported by The Netherlands Organization for Scientific Research (NWO) and is part of the Dutch Astrochemistry Network (DAN) II (Project No. 648.000.029). PE-J, SM, and JP acknowledge support from the Swedish Research Council and the Swedish Foundation for Strategic Research. The authors are additionally thankful for the support from the following funding bodies: the UK EPSRC (MBR and CV-EP/L005913/1 and EP/V026690/1; MBU-EP/S028617/1), STFC (PNPAS award and mini-IPS Grant No. ST/J002895/1), the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, US Department of Energy (FZ—DE-FG02-86ER13491); the National Science Foundation (DR - PHYS-1753324); and the Helmholtz Initiative and Networking Fund through the Young Investigators Group Program (SB). We acknowledge the use of the Maxwell computational resources operated at Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany.

Publisher Copyright:
Copyright © 2022 Garg, Lee, Tikhonov, Chopra, Steber, Lemmens, Erk, Allum, Boll, Cheng, Düsterer, Gruet, He, Heathcote, Johny, Kazemi, Köckert, Lahl, Loru, Maclot, Mason, Müller, Mullins, Olshin, Passow, Peschel, Ramm, Rompotis, Trippel, Wiese, Ziaee, Bari, Burt, Küpper, Rijs, Rolles, Techert, Eng-Johnsson, Brouard, Vallance, Manschwetus and Schnell.

Keywords

  • free electron laser
  • polycylic aromatic hydrocarbon (PAH)
  • time-resolved spectroscopy
  • ultrafast dynamics of molecules
  • velocity-map imaging mass spectrometry

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