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Polycyclic aromatic hydrocarbon (PAH) dimers are crucial for soot nucleation. This study predicts PAH dimer fluorescence, confirming their potential role in flame diagnostics and soot formation.

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Area of Science:

  • Combustion Chemistry
  • Physical Chemistry
  • Spectroscopy

Background:

  • Polycyclic aromatic hydrocarbons (PAHs) are key intermediates in soot formation.
  • PAH dimerization is hypothesized to be critical in soot nucleation, but experimental evidence is limited.
  • Laser-induced fluorescence (LIF) is a potential in situ diagnostic for identifying PAH dimers in flames.

Purpose of the Study:

  • To computationally investigate the excited-state properties and fluorescence emission of PAH dimers (excimers and exciplexes).
  • To determine if theoretical models can predict the fluorescence characteristics of PAH dimers relevant to experimental observations.
  • To assess the role of PAH dimer fluorescence in flame diagnostics.

Main Methods:

  • Utilized nonempirically tuned LC-BLYP functionals for accurate electronic structure calculations.
  • Computed excited-state geometries and emission energies for a diverse database of 81 PAH excimers and exciplexes.
  • Analyzed the relationship between monomer properties and exciplex emission energies.

Main Results:

  • Calculated emission energies for PAH excimers and exciplexes show dependence on PAH topology.
  • A linear correlation was found between mean monomer bandgap and computed exciplex emission energy.
  • The predicted fluorescence energy range for small to medium PAHs aligns with experimental LIF observations.

Conclusions:

  • PAH excimer and exciplex fluorescence is theoretically predictable and can be distinguished from monomers.
  • The findings support the potential use of LIF for detecting PAH dimers in flames.
  • This research provides a theoretical basis for understanding PAH dimer contributions to soot nucleation and flame diagnostics.