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Electron-nuclear wave-packet dynamics through a conical intersection.

Kilian Hader1, Julian Albert1, E K U Gross2

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Electron-nuclear dynamics near conical intersections (CoIns) were studied. Results show nuclear and electronic densities remain unchanged during population transfer, contrary to adiabatic state analysis.

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Area of Science:

  • Quantum dynamics
  • Theoretical chemistry
  • Molecular physics

Background:

  • Conical intersections (CoIns) are critical points in molecular potential energy surfaces where electronic states become degenerate.
  • Understanding electron-nuclear coupling dynamics at CoIns is essential for describing non-adiabatic processes like photochemical reactions.
  • Adiabatic state analysis often predicts significant changes in nuclear and electronic densities at CoIns.

Purpose of the Study:

  • To investigate the coupled electron-nuclear dynamics in a model system exhibiting a conical intersection.
  • To compare the dynamics of nuclear and electronic densities with predictions from adiabatic state analysis.
  • To elucidate the behavior of wave packets traversing a conical intersection.

Main Methods:

  • A two-dimensional model system with one electron and one nucleus was employed.
  • The system evolved under an external static field.
  • Coupled electron-nuclear wave packet dynamics were simulated.

Main Results:

  • Nuclear density conserved its initial Gaussian shape when passing the conical intersection.
  • Electronic density remained approximately constant during passage through the CoIn.
  • These observations contrasted sharply with dramatic changes predicted by adiabatic electronic state analysis.

Conclusions:

  • Neither nuclear nor electronic densities are significantly influenced by the conical intersection during efficient population transfer.
  • The nuclear-electronic wave packet moves on a smooth, complete potential energy surface, explaining the lack of density changes.
  • This finding challenges traditional views derived from adiabatic approximations in describing dynamics at CoIns.