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This study introduces a novel simulation method combining quantum and classical approaches to model open quantum systems, specifically polaritons. The new method accurately captures dissipation effects, revealing their impact on chemical reactions.

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Area of Science:

  • Quantum dynamics
  • Physical chemistry
  • Computational physics

Background:

  • Polaritons, formed by hybridizing matter and photons, are open quantum systems due to finite photon lifetimes.
  • Accurately simulating nonadiabatic processes in these systems requires accounting for dissipation.

Purpose of the Study:

  • To develop and test a novel simulation method for nonadiabatic dynamics in open quantum systems with dissipation.
  • To investigate the influence of polariton dissipation on chemical reaction dynamics.

Main Methods:

  • Combined Schrödinger-Langevin equation with split-operator Fourier transform.
  • Employed mixed quantum-classical methods: Ehrenfest dynamics and fewest-switches surface hopping.
  • Tested on spontaneous emission, Tully-I model with dissipation, and a lossy cavity isomerization model.

Main Results:

  • The developed method consistently reproduced results across different test cases.
  • Demonstrated that polariton dissipation significantly alters isomerization reaction pathways.
  • Validated the accuracy and applicability of the combined simulation approach.

Conclusions:

  • The novel simulation approach effectively models nonadiabatic dynamics in open quantum systems with dissipation.
  • This method offers a valuable tool for studying polariton behavior and its influence on chemical processes.
  • Potential for broad applications in quantum dynamics and related scientific fields.