Ultrafast dynamics of fluorene initiated by highly intense laser fields

12 February 2024, Version 2
This content is a preprint and has not undergone peer review at the time of posting.

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.

Keywords

ultrafast dynamics
strong-field ionization
fragmentation
polycyclic aromatic hydrocarbons
molecular dynamics
covariance analysis
global fitting

Supplementary materials

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Description
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Electronic Supporting Information
Description
This PDF contains fitting results, additional images and data, and detailed descriptions of various analysis and simulation details.
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Dataset
Description
A *.tar.xz archive with fitting files, and raw data for the figures.
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