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Electron Transfer in Frozen Media.

Pingyun Chen1, Thomas J. Meyer

  • 1Department of Chemistry, The University of North Carolina, Chapel Hill, North Carolina 27599-3290.

Inorganic Chemistry
|September 11, 1996
PubMed
Summary

Electron transfer theories are updated for rigid media, showing solvent effects alter activation energy. This impacts photoinduced electron transfer and excited state interconversions in non-fluid environments.

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Isolation and Characterization of the Osmium(V)-Imido Complex [Os(V)(Tp)(Cl)(2)(NH)] We are grateful to the National Science Foundation under Grant number CHE-9503738, the Los Alamos National Laboratory (DOE) under Grant Number 10730-001-00-2C, and the Laboratory Directed Research and Development Program for support of this research. M. H. V. Huynh gratefully acknowledges postdoctoral fellowship support from the Directorapos;s Office of Los Alamos National Laboratory. Los Alamos National Laboratory is operated by the University of California for the U.S. Department of Energy under Contract W-7405-ENG-36. We also thank Dr. Paul R. Sharp (Professor of Chemistry, University of Missouri, Columbia, MO, 65211) for the information on transition metal parent imido complexes.

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Medium Effects on Charge Transfer in Metal Complexes.

Chemical reviews·2002

Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Molecular Dynamics

Background:

  • Classical electron transfer theories primarily consider fluid media.
  • Solvent reorganization energy is a key factor influencing electron transfer rates.
  • Understanding electron transfer in different media is crucial for chemical and physical processes.

Purpose of the Study:

  • To modify classical electron transfer theories for rigid media.
  • To analyze the impact of frozen solvent polarization on electron transfer.
  • To investigate photoinduced electron transfer and excited state interconversions in rigid environments.

Main Methods:

  • Theoretical modification of classical electron transfer models.
  • Analysis of dynamic intramolecular vibrations and dielectric polarization in rigid media.
  • Examination of solvent reorganizational energy and activation free energy changes.

Main Results:

  • In rigid media, electron transfer occurs with a 'frozen' solvent orientation from the initial state.
  • This 'frozen' solvent leads to increased free energy change and decreased solvent reorganizational energy.
  • Activation free energy for electron transfer increases in rigid media compared to fluid media.

Conclusions:

  • Electron transfer theories must account for the unique solvent dynamics in rigid media.
  • Rigid media significantly alter the energetics and kinetics of electron transfer processes.
  • The developed analysis framework is applicable to photoinduced electron transfer and excited state dynamics.

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