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A classical ride through a conical intersection.

Thomas Schaupp1, Volker Engel1

  • 1Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Emil-Fischer-Str. 42, 97074 Würzburg, Germany.

The Journal of Chemical Physics
|January 21, 2019
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Summary
This summary is machine-generated.

Classical and quantum dynamics near conical intersections (CoIns) were studied. Classical trajectories in full phase space track quantum wave packets through CoIns, enabling non-adiabatic population transfer.

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Area of Science:

  • Quantum dynamics
  • Chemical physics
  • Theoretical chemistry

Background:

  • Conical intersections (CoIns) are crucial for non-adiabatic processes in molecular systems.
  • Understanding electron-nuclear motion near CoIns is key to predicting chemical reaction pathways.
  • Previous studies have explored quantum and classical descriptions of molecular dynamics.

Purpose of the Study:

  • To investigate the correlated electron-nuclear motion in a model system near a conical intersection.
  • To compare quantum wave-packet dynamics with classical trajectory simulations.
  • To analyze population transfer during non-adiabatic transitions.

Main Methods:

  • Simulating the dynamics of a model system in the vicinity of a conical intersection.
  • Employing an ensemble of classical trajectories in the complete electronic-nuclear phase space.
  • Analyzing quantum wave-packet motion and population transfer.
  • Comparing with adiabatic circular motion and Born-Oppenheimer classical nuclear motion.

Main Results:

  • Classical trajectories in the full electronic-nuclear phase space accurately track quantum wave-packet motion through the CoIn.
  • Non-adiabatic population transfer is observed during this process.
  • For adiabatic circular motion, significant deviations occur between quantum and classical densities.
  • Born-Oppenheimer classical nuclear motion on a single potential surface can track quantum dynamics in specific adiabatic cases.

Conclusions:

  • Classical dynamics in the complete phase space provide a viable method for describing quantum wave-packet motion through conical intersections.
  • The choice of classical approximation significantly impacts the accuracy of simulating non-adiabatic dynamics.
  • This work offers insights into the quantum-classical correspondence in regions of strong electronic-nuclear coupling.