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Electron-Induced Proton Transfer.

Dmitry V Matyushov1, Marshall D Newton2

  • 1School of Molecular Sciences and Department of Physics, Arizona State University, P.O. Box 871504, Tempe, Arizona 85287-1504, United States.

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|October 29, 2021
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Summary
This summary is machine-generated.

Electron transfer can trigger activationless proton transfer by creating a highly polarized environment. This process, occurring on a picosecond timescale, dynamically alters charge screening and is influenced by medium relaxation dynamics.

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Theoretical Chemistry

Background:

  • Electron transfer reactions are fundamental in chemistry and biology.
  • Proton transfer is often coupled to electron transfer events.
  • The role of medium polarization in mediating proton transfer is crucial.

Purpose of the Study:

  • To theoretically investigate the mechanism of activationless proton transfer.
  • To elucidate the influence of electron transfer on proton transfer dynamics.
  • To analyze the impact of medium polarization and reorganization energy.

Main Methods:

  • Theoretical study of electron-induced proton transfer.
  • Analysis of nonequilibrium medium polarization effects.
  • Calculation of cross electron-proton reorganization energy.
  • Investigation of medium relaxation dynamics and de Gennes narrowing.

Main Results:

  • Electron transfer induces highly nonequilibrium medium polarization, driving activationless proton transfer.
  • Cross electron-proton reorganization energy is a key parameter, dependent on electron-proton distances and pKa differences.
  • Medium relaxation occurs on the (sub)picosecond timescale, defining the proton transfer time.
  • Microscopic calculations show slower collective relaxation than continuum models.

Conclusions:

  • Activationless proton transfer is a viable pathway initiated by electron transfer.
  • Medium polarization plays a critical role in modulating proton transfer rates.
  • The theoretical framework provides insights into charge transfer processes in condensed phases.