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Area of Science:

  • Quantum dynamics
  • Photochemistry
  • Molecular spectroscopy

Background:

  • Ultrafast dynamics in complex quantum systems require accessing coherences.
  • Conical intersections in photochemical processes generate electronic coherences.
  • Spin-orbit coupling significantly influences molecular electronic structures.

Purpose of the Study:

  • To investigate the persistence of electronic coherences in spin-orbit-split states after molecular dissociation.
  • To quantify the transfer of coherence magnitude from molecular to atomic regimes.
  • To propose a novel experimental technique for observing and controlling these coherences.

Main Methods:

  • Accurate quantum mechanical calculations on gas-phase methyl iodide.
  • Simulation of photochemical dissociation dynamics.
  • Development and proposal of heterodyned attosecond four-wave-mixing spectroscopy.

Main Results:

  • Electronic coherences of spin-orbit-split states persist in atomic iodine post-dissociation.
  • A maximum of 0.75% vibronic coherence was predicted in the molecular phase.
  • One-third of the molecular coherence magnitude transfers to a long-lived atomic coherence.

Conclusions:

  • Electronic coherences can survive molecular dissociation, transferring to atomic fragments.
  • Heterodyned attosecond four-wave-mixing spectroscopy can resolve and reconstruct these coherences.
  • This technique offers a pathway to control spin-orbit-coupled electronic states in photochemistry.