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This study introduces a new method to analyze rare reactive pathways in open quantum systems. It reveals how system geometry influences quantum dynamics and relaxation mechanisms.

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Area of Science:

  • Quantum dynamics
  • Chemical physics
  • Theoretical chemistry

Background:

  • Studying rare reactive pathways in open quantum systems is challenging.
  • Dissipative and nonadiabatic dynamics require advanced theoretical frameworks.
  • Understanding quantum processes in Markovian environments is crucial.

Purpose of the Study:

  • To develop a method for studying rare reactive pathways in open quantum systems.
  • To elucidate reactive paths for dissipative, nonadiabatic dynamics.
  • To analyze the influence of system geometry on quantum dynamics and relaxation.

Main Methods:

  • Utilizing transition path theory.
  • Employing ensembles of quantum jump trajectories.
  • Analyzing a minimal model of a conical intersection.

Main Results:

  • Identified dominant pathways and rates for thermally activated processes.
  • Detailed relaxation pathways and photoyields following vertical excitation.
  • Found that conical intersection geometry affects transition state electronic character and relaxation mechanisms.

Conclusions:

  • The developed approach generalizes classical reactive path concepts to quantum processes.
  • Conical intersection geometry plays a critical role in nonadiabatic dynamics.
  • The study provides insights into pathways dominated by dephasing versus dissipation.