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This study introduces off-diagonal quantum master equations (OD-QMEs) for modeling charge transfer (CT) dynamics in complex molecules with time-dependent couplings. It shows how external fields can modify CT pathways and kinetics, particularly under high temperatures.

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Area of Science:

  • Chemical Physics
  • Quantum Dynamics
  • Molecular Modeling

Background:

  • Off-diagonal quantum master equations (OD-QMEs) are valuable for modeling charge transfer (CT) dynamics.
  • Existing OD-QMEs often assume time-independent electronic couplings, limiting their application to complex, driven systems.

Purpose of the Study:

  • To develop and analyze OD-QMEs for molecular systems with time-dependent electronic couplings.
  • To investigate the influence of external fields on CT dynamics and kinetics.
  • To demonstrate the potential for off-diagonal driving to create new CT pathways.

Main Methods:

  • Formulation of OD-QMEs for systems with time-dependent electronic coupling terms.
  • Asymptotic analysis of OD-QME dynamics under continuous wave (CW) field driving.
  • Application to the Garg-Onuchic-Ambegaokar CT model.

Main Results:

  • The developed OD-QMEs accurately describe CT dynamics in systems driven by time-dependent external fields.
  • Asymptotic analysis reveals a transition to rate kinetics governed by field-modified Marcus theory constants at long times and high temperatures.
  • Off-diagonal driving was shown to enable new CT pathways that compete with non-radiative decay.

Conclusions:

  • The presented OD-QMEs provide a robust framework for studying driven CT dynamics.
  • External fields can significantly alter CT pathways and kinetics, offering new avenues for controlling molecular processes.
  • This approach enhances our understanding of charge transfer in complex molecular systems under external influence.