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Updated: Dec 30, 2025

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
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Dissipation and dynamics in ultrafast intersystem crossings.

Michel van Veenendaal1

  • 1Department of Physics, Northern Illinois University, DeKalb, Illinois 60115, USA.

The Journal of Chemical Physics
|January 17, 2020
PubMed
Summary

Ultrafast intersystem crossings are affected by dynamics and dissipation. Standard methods like Fermi's golden rule are limited, showing deviations in population transfer rates.

Area of Science:

  • Quantum dynamics
  • Chemical physics
  • Spectroscopy

Background:

  • Ultrafast intersystem crossing (UISC) is crucial in photochemistry and photophysics.
  • Understanding UISC in dissipative systems is essential for controlling molecular processes.
  • Standard models often simplify system-environment interactions.

Purpose of the Study:

  • To investigate the impact of dynamics and dissipation on UISC.
  • To develop and apply an improved wave packet propagation method.
  • To assess the limitations of Fermi's golden rule for rate calculations.

Main Methods:

  • Simulating a dissipative two-level system coupled to a vibronic mode.
  • Employing an amplitude damping method for wave packet propagation.

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  • Comparing simulation results with Fermi's golden rule predictions.

    • Main Results:

    • Dynamics and dissipation significantly alter UISC rates and times.
    • Deviations from exponential population transfer are observed.
    • Wave packet recurrence ('spill back') is a notable phenomenon.
    • Fermi's golden rule is shown to be applicable only under specific conditions.

    Conclusions:

    • Standard theoretical approaches may not fully capture UISC in complex systems.
    • Accurate modeling requires accounting for system dynamics and dissipation.
    • The developed amplitude damping method offers improved accuracy.