Ultrafast dynamics of fluorene initiated by highly intense laser fields

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

doi:10.1039/D3CP05063G

Ultrafast dynamics of fluorene initiated by highly intense laser fields†

Diksha Garg,^ab Pragya Chopra,^ac Jason W. L. Lee,

^ad Denis S. Tikhonov,

^a Sonu Kumar,

^ab Oender Akcaalan,^a Felix Allum,

‡§^d Rebecca Boll,

^e Alexander A. Butler,^d Benjamin Erk,

^a Eva Gougoula,

^a Sébastien P. Gruet,^a Lanhai He,

^f David Heathcote,

^d Ellen Jones,^d Mehdi M. Kazemi,^a Jan Lahl,^g Alexander K. Lemmens,

^hi Zhihao Liu,^d Donatella Loru,

^a Sylvain Maclot,

^j Robert Mason,^d James Merrick,^d Erland Müller,^a Terry Mullins,^fe Christina C. Papadopoulou,^a Christopher Passow,^a Jasper Peschel,^g Marius Plach,

^g Daniel Ramm,^a Patrick Robertson,

¶^d Dimitrios Rompotis,

^ae Alcides Simao,

||^a Amanda L. Steber,

**^a Ayhan Tajalli,

^a Atia Tul-Noor,

^a Nidin Vadassery,^fk Ivo S. Vinklárek,^f Simone Techert,^a Jochen Küpper,

^fblk Anouk M. Rijs,

^m Daniel Rolles,

ⁿ Mark Brouard,

^d Sadia Bari,

^ao Per Eng-Johnsson,

^g Claire Vallance,

^d Michael Burt,

^d Bastian Manschwetus

††^a and Melanie Schnell

*^ac

Author affiliations

* Corresponding authors

^a Deutsches Elektronen-Synchrotron DESY, Hamburg, Germany
E-mail: melanie.schnell@desy.de

^b Department of Physics, Universität Hamburg, Hamburg, Germany

^c Institute of Physical Chemistry, Christian-Albrechts-Universität zu Kiel, Kiel, Germany

^d Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Oxford, UK

^e European XFEL, Schenefeld, Germany

^f Center for Free-Electron Laser Science CFEL, Deutsches Elektronen-Synchrotron DESY, Germany

^g Department of Physics, Lund University, Lund, Sweden

^h Van’t Hoff Institute for Molecular Sciences, University of Amsterdam, Amsterdam, The Netherlands

ⁱ FELIX Laboratory, Radboud University, Nijmegen, The Netherlands

^j Université Claude Bernard Lyon 1, Villeurbanne, France

^k Department of Chemistry, Universität Hamburg, Hamburg, Germany

^l Center for Ultrafast Imaging, Universität Hamburg, Hamburg, Germany

^m Division of BioAnalytical Chemistry, Vrije Universiteit Amsterdam, Amsterdam, The Netherlands

ⁿ J. R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, KS, USA

^o Zernike Institute for Advanced Materials, University of Groningen, Groningen, The Netherlands

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.

This article is part of the themed collection: Molecular Dynamics in the Gas Phase

Physical Chemistry Chemical Physics

Ultrafast dynamics of fluorene initiated by highly intense laser fields†

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