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Area of Science:

  • Astrochemistry
  • Photochemistry
  • Quantum Chemistry

Background:

  • Methaniminium cation (CH2NH2+) is crucial for Titan's atmospheric chemistry.
  • It models the retinal protonated Schiff base (PSB) in vertebrate vision.
  • Previous studies focused on CN bond cleavage and photoisomerization of CH2NH2+.

Purpose of the Study:

  • To investigate novel UV-induced photochemical pathways of the methaniminium cation.
  • To identify new reaction channels beyond CN bond cleavage and photoisomerization.
  • To understand the formation of HCNH+ in Titan's atmosphere.

Main Methods:

  • High-level ab initio calculations (XMCQDPT2 and CASSCF(12,12)).
  • On-the-fly trajectory surface hopping dynamics simulations.
  • Machine learning-accelerated simulations for large-scale dynamics.

Main Results:

  • A new photochemical pathway yielding HCNH+ from CH2NH2+ via double H atom elimination was identified.
  • A novel S1/S0 conical intersection mediating this pathway was characterized.
  • Direct H2 loss was confirmed following S2 or S1 excitation.
  • Mode-specific pre-excitation was shown to selectively control this new photochemical channel.

Conclusions:

  • The study reveals a previously unknown photochemical route for CH2NH2+ relevant to Titan's atmosphere.
  • This discovery offers insights into the nonadiabatic dynamics of PSBs.
  • Targeted control of photochemical outcomes is achievable through vibrational mode excitation.