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Area of Science:

  • Chemical Physics
  • Molecular Dynamics
  • Spectroscopy

Background:

  • Ultrafast x-ray sources enable probing of complex molecular dynamics.
  • Non-Born-Oppenheimer effects, governed by conical intersections, are crucial in excited-state molecular behavior.

Purpose of the Study:

  • To investigate the dynamics of photoexcited ethylene using advanced x-ray spectroscopies.
  • To demonstrate the sensitivity of time-resolved x-ray absorption (TRXAS) to molecular electronic-nuclear dynamics.

Main Methods:

  • High-level ab initio quantum dynamics simulations.
  • Time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) were employed.
  • Study focused on ethylene excited to the S₂(ππ*) state.

Main Results:

  • TRXAS and TRXPS provided clear signatures of wave packet dynamics near conical intersections.
  • Observed charge localization effects driven by nuclear dynamics were identified.
  • TRXAS proved highly sensitive to the molecular dynamics following photoexcitation.

Conclusions:

  • Ultrafast x-ray spectroscopies are powerful tools for observing dynamics around conical intersections.
  • These techniques offer a direct route to studying charge localization in excited-state dynamics.
  • The findings highlight the potential of x-ray methods in understanding fundamental molecular processes.