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Donor-Bridge-Acceptor Proton Transfer in Aqueous Solution.

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Proton transfer in water involves a rapid "through bridge" mechanism, forming hydronium structures. Other configurations act as dead ends, highlighting the complexity of charge transfer in aqueous systems.

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Eigen intermediateZundel formab initio molecular dynamicsacid−base reactioncharge transferconcerted mechanism

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Area of Science:

  • Physical Chemistry
  • Computational Chemistry
  • Chemical Physics

Background:

  • Proton transfer is fundamental to many chemical and biological processes.
  • Understanding proton transfer mechanisms in aqueous environments is crucial.

Purpose of the Study:

  • To investigate the dynamics of proton transfer in a donor-bridge-acceptor system using a single water molecule as the bridge.
  • To elucidate the dominant pathways and structural configurations involved in charge transfer within an aqueous solution.

Main Methods:

  • Ab initio molecular dynamics simulations were employed.
  • A large number of proton transfer trajectories were analyzed.
  • The system comprised a donor-bridge-acceptor setup embedded in aqueous solution.

Main Results:

  • The dominant charge transfer pathway is a subpicosecond "through bridge" event.
  • The water bridge adopts an Eigen-like (hydronium) structure during dominant proton transfer.
  • A Zundel-like configuration was identified as a potential dead end for charge transfer.

Conclusions:

  • Proton transfer in this system is a rapid, multidimensional process.
  • The reaction coordinate cannot be simplified to local structural or solvent parameters.
  • The study reveals key insights into the molecular mechanisms of proton transfer in water.