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Title: Ultrafast dynamics of fluorene initiated by highly intense laser fields

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI: https://doi.org/10.1039/d3cp05063g · OSTI ID:2446552
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  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany); SLAC
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Christian-Albrechts-Universität zu Kiel (Germany)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Oxford (United Kingdom)
  4. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
  6. Univ. of Oxford (United Kingdom); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  7. European XFEL, Schenefeld (Germany)
  8. Univ. of Oxford (United Kingdom)
  9. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science
  10. Lund Univ. (Sweden)
  11. Univ. of Amsterdam (Netherlands); Radboud Univ., Nijmegen (Netherlands)
  12. Université Claude Bernard Lyon, Villeurbanne (France)
  13. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science; European XFEL, Schenefeld (Germany)
  14. Univ. of Oxford (United Kingdom); Univ. of Nottingham (United Kingdom)
  15. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); European XFEL, Schenefeld (Germany)
  16. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Ruhr Univ., Bochum (Germany)
  17. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Universidad de Valladolid (Spain)
  18. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany). Center for Free-Electron Laser Science; Univ. of Hamburg (Germany)
  19. Vrije Univ., Amsterdam (Netherlands)
  20. Kansas State Univ., Manhattan, KS (United States)
  21. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Groningen (Netherlands)
  22. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Class 5 Photonics, Hamburg (Germany)

Here, 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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
Engineering and Physical Sciences Research Council (EPSRC); Federal Ministry of Education and Research (BMBF); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
2446552
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 30 Vol. 26; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (54)

Towards First Principles Calculation of Electron Impact Mass Spectra of Molecules journal April 2013
Hydrogen Abstraction/Acetylene Addition Revealed journal June 2014
Extended tight‐binding quantum chemistry methods journal August 2020
Monitoring of environmental exposure to polycyclic aromatic hydrocarbons: a review journal November 2007
Ionisation and fragmentation of polycyclic aromatic hydrocarbons by femtosecond laser pulses at wavelengths resonant with cation transitions journal July 2002
Detailed modeling of soot particle nucleation and growth journal January 1991
Ionisation and fragmentation dynamics of laser desorbed polycyclic aromatic hydrocarbons using femtosecond and nanosecond post-ionisation journal September 2002
GFN2-xTB—An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions journal January 2019
Interplay of Open-Shell Spin-Coupling and Jahn–Teller Distortion in Benzene Radical Cation Probed by X-ray Spectroscopy journal October 2020
Table-Top X-ray Spectroscopy of Benzene Radical Cation journal October 2020
Smallest Organic Tetracation in the Gas Phase: Stability of Multiply Charged Diiodoacetylene Produced in Intense Femtosecond Laser Fields journal September 2021
How to Compute Electron Ionization Mass Spectra from First Principles journal May 2016
Calculation of Electron Ionization Mass Spectra with Semiempirical GFNn-xTB Methods journal September 2019
Hydrogen Abstraction Acetylene Addition and Diels−Alder Mechanisms of PAH Formation:  A Detailed Study Using First Principles Calculations journal September 2005
Effects of Polarization of 1.4 μm Femtosecond Laser Pulses on the Formation and Fragmentation of Naphthalene Molecular Ions Compared at the Same Effective Ionization Intensity journal October 2005
Formation and Fragmentation of Quadruply Charged Molecular Ions by Intense Femtosecond Laser Pulses journal June 2010
Multimass Velocity-Map Imaging with the Pixel Imaging Mass Spectrometry (PImMS) Sensor: An Ultra-Fast Event-Triggered Camera for Particle Imaging journal November 2012
XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment journal August 2015
Atomic excitation during recollision-free ultrafast multi-electron tunnel ionization journal May 2006
Electron correlation driven non-adiabatic relaxation in molecules excited by an ultrashort extreme ultraviolet pulse journal January 2019
Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast XUV-IR regime journal October 2021
Ultrafast dynamics of correlation bands following XUV molecular photoionization journal November 2020
A localized view on molecular dissociation via electron-ion partial covariance journal March 2022
Predicting Coulomb explosion fragment angular distributions using molecular ground-state vibrational motion journal January 2022
Polycyclic aromatic hydrocarbon processing by cosmic rays journal December 2010
Pure hydrocarbon cycles in TMC-1: Discovery of ethynyl cyclopropenylidene, cyclopentadiene, and indene journal May 2021
Search for far-IR PAH bands with Herschel: modelling and observational approaches journal January 2011
Photoelectron imaging spectrometry: Principle and inversion method journal June 1996
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal September 1997
On the Correlation Problem in Atomic and Molecular Systems. Calculation of Wavefunction Components in Ursell‐Type Expansion Using Quantum‐Field Theoretical Methods journal December 1966
Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen journal January 1989
Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions journal May 1992
Photoelectron and photofragment velocity map imaging of state-selected molecular oxygen dissociation/ionization dynamics journal August 1997
Three-dimensional imaging of carbonyl sulfide and ethyl iodide photodissociation using the pixel imaging mass spectrometry camera journal October 2015
Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera journal July 2017
Coulomb explosion imaging of CH 3 I and CH 2 ClI photodissociation dynamics journal November 2018
A direct comparison of high-speed methods for the numerical Abel transform journal June 2019
The ORCA quantum chemistry program package journal June 2020
Femtosecond real-time probing of reactions XXII. Kinetic description of probe absorption, fluorescence, depletion and mass spectrometry journal December 1996
Coincidence and covariance data acquisition in photoelectron and -ion spectroscopy. I. Formal theory journal October 2013
Polycyclic Aromatic Hydrocarbon Contribution to the Infrared Output Energy of the Universe at z ≃ 2 journal September 2004
Above-threshold ionisation journal October 1988
FLASH—the first soft x-ray free electron laser (FEL) user facility journal September 2010
Covariance mapping techniques journal July 2016
Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene in strong IR and UV laser fields journal November 2015
Covariance imaging experiments using a pixel-imaging mass-spectrometry camera journal January 2014
Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera journal May 2015
Transition from nonsequential to sequential double ionization in many-electron systems journal September 2017
Above-threshold ionization with subpicosecond laser pulses journal September 1987
CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser journal August 2018
Photoelectron energy peaks shift against the radiation pressure in strong-field ionization journal March 2022
“The Even-Lavie valve as a source for high intensity supersonic beam” journal December 2015
The Smallest Aromatic Tetracation Produced in Gas Phase by Intense Femtosecond Laser Pulses journal December 2019
Discovery of the Pure Polycyclic Aromatic Hydrocarbon Indene (c-C9H8) with GOTHAM Observations of TMC-1 journal May 2021

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