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Area of Science:

  • Chemical Physics
  • Photochemistry
  • Molecular Dynamics

Background:

  • o-nitrophenol photolysis is a potential atmospheric source of nitrous acid.
  • Previous studies focused on photolysis products and electronic dynamics, not ultrafast nuclear motions.
  • The intramolecular proton transfer during non-radiative relaxation remains experimentally unresolved.

Purpose of the Study:

  • To directly observe the ultrafast nuclear dynamics of o-nitrophenol during photo-relaxation.
  • To spatiotemporally resolve the key steps in the non-radiative decay pathway.
  • To elucidate the mechanism of proton transfer-mediated relaxation.

Main Methods:

  • Ultrafast electron diffraction (UED) was employed for direct observation.
  • Ab initio multiple spawning (AIMS) simulations were used for theoretical support.
  • Femtosecond timescale and sub-Angstrom resolution were achieved.

Main Results:

  • Direct observation of ultrafast nuclear motions mediating photo-relaxation.
  • Spatiotemporal resolution of the loss of planarity after proton transfer.
  • Identification of access to a conical intersection between excited and ground states.

Conclusions:

  • The study provides the first experimental resolution of nuclear dynamics in o-nitrophenol relaxation.
  • Insights into the proton transfer and subsequent loss of planarity mechanism were gained.
  • This work advances understanding of photochemical processes in atmospheric chemistry.