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Relaxation dynamics through a conical intersection: Quantum and quantum-classical studies.

Carlotta Pieroni1, Emanuele Marsili2, David Lauvergnat1

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Investigating the photo-excited retinal chromophore relaxation, this study compares quantum-classical dynamics with exact quantum wavepacket dynamics. Initial condition sampling significantly impacts nonadiabatic dynamics simulations for rhodopsin

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Area of Science:

  • Theoretical Chemistry
  • Photochemistry
  • Molecular Dynamics

Background:

  • Rhodopsin's visual cycle involves the photo-isomerization of the retinal chromophore.
  • Understanding this process requires modeling nonadiabatic dynamics through conical intersections.
  • A minimal two-electronic-state, two-dimensional Hamiltonian models key features of retinal isomerization.

Purpose of the Study:

  • To analyze the relaxation dynamics of a photo-excited retinal chromophore model.
  • To evaluate the performance of trajectory-based schemes for nonadiabatic dynamics.
  • To investigate the impact of initial condition sampling on dynamics simulations.

Main Methods:

  • Utilized a two-electronic-state, two-dimensional Hamiltonian based on Hahn and Stock.
  • Compared quantum-classical trajectory simulations with numerically exact quantum vibronic wavepacket dynamics.
  • Analyzed electronic and nuclear observables to assess dynamics.

Main Results:

  • Quantum-classical methods were compared against exact quantum dynamics for accuracy.
  • The influence of initial condition sampling on simulation outcomes was investigated.
  • Performance of various nonadiabatic dynamics schemes was evaluated.

Conclusions:

  • Initial condition sampling is a critical factor affecting the accuracy of nonadiabatic dynamics simulations.
  • The study provides insights into the dynamics of photo-excited retinal chromophores.
  • Findings aid in refining computational models for photochemical processes.