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Solvent friction effect on intramolecular electron transfer.

Min Liu1, Naoki Ito, Mark Maroncelli

  • 1Department of Chemistry, Pennsylvania State University, University Park, Pennsylvania 16802, USA.

Journal of the American Chemical Society
|December 15, 2005
PubMed
Summary

Electron transfer rates in U-shaped molecules depend on temperature and solvent properties. At high temperatures, nonadiabatic models apply, while solvent friction dominates at low temperatures, altering the electron transfer mechanism.

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Materials Science

Background:

  • U-shaped donor-bridge-acceptor molecules are crucial for understanding electron transfer processes.
  • Solvent dynamics significantly influence charge transfer reactions.
  • Previous studies have explored electron transfer in various solvent environments.

Purpose of the Study:

  • To investigate the temperature-dependent electron transfer rates in U-shaped molecules.
  • To examine the role of slow-relaxing solvents like N-methylacetamide (NMA) and N-methylpropionamide (NMP).
  • To elucidate the transition in electron transfer mechanisms at different temperatures.

Main Methods:

  • Experimental investigation of electron transfer rates as a function of temperature.
  • Utilizing solvents with slow polarization relaxation dynamics.
  • Comparison of experimental data with theoretical nonadiabatic and solvent friction models.

Main Results:

  • At high temperatures, electron transfer rates align with nonadiabatic theoretical predictions.
  • At low temperatures, solvent friction becomes the dominant factor controlling electron transfer rates.
  • A clear shift in the electron transfer mechanism is observed with changing temperature.

Conclusions:

  • The study reveals a temperature-induced transition in electron transfer mechanisms.
  • Solvent friction plays a critical role in governing electron transfer at low temperatures.
  • Findings provide insights into controlling charge transfer in molecular systems.