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Electron transfer in confined electromagnetic fields.

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Cavity quantum electrodynamics enhances molecular electron transfer rates. Coupling to cavity modes boosts electron transfer in the Marcus inverted region, offering control via plasmonics.

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Area of Science:

  • Quantum physics
  • Molecular electronics
  • Nanophotonics

Background:

  • Cavity quantum electrodynamics (cQED) explores light-matter interactions.
  • Nanophotonics enables control over light at the nanoscale.
  • Electron transfer is crucial in molecular systems.

Purpose of the Study:

  • To investigate nonadiabatic electron transfer in a confined cavity field.
  • To develop a generalized framework for molecular-cavity interactions.
  • To explore rate enhancement in electron transfer processes.

Main Methods:

  • Developed a generalized Hamiltonian for charged molecular systems and quantized cavity fields.
  • Applied the framework to donor-acceptor electron transfer within a cavity.
  • Analyzed two limiting cases: fast and slow electron tunneling relative to the cavity mode.

Main Results:

  • The effective system Hamiltonian unifies Rabi and spin-boson models with a self-dipole term.
  • Significant electron transfer rate enhancement observed in the Marcus inverted region.
  • Coupling to the cavity mode is shown to be a key factor in rate enhancement.

Conclusions:

  • Coupling molecular systems to cavity modes offers a pathway to control electron transfer.
  • Visible and infrared plasmonics can be utilized to manipulate electron transfer processes.
  • This work opens new avenues for designing molecular electronic devices.