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Yao Wang, Yu Su, Ruixue Xu, Xiao Zheng, Yijing Yan. Marcus' electron transfer rate revisited via a Rice-Ramsperger-Kassel-Marcus analogue: A unified formalism for linear and nonlinear solvation scenarios[J]. Chinese Journal of Chemical Physics .
Citation: Yao Wang, Yu Su, Ruixue Xu, Xiao Zheng, Yijing Yan. Marcus' electron transfer rate revisited via a Rice-Ramsperger-Kassel-Marcus analogue: A unified formalism for linear and nonlinear solvation scenarios[J]. Chinese Journal of Chemical Physics .

Marcus' electron transfer rate revisited via a Rice-Ramsperger-Kassel-Marcus analogue: A unified formalism for linear and nonlinear solvation scenarios

  • Received Date: 2021-01-05
  • Accepted Date: 2021-01-26
  • Rev Recd Date: 2021-01-22
  • Available Online: 2021-02-04
  • In the pioneering work by R. A. Marcus, the solvation effect on electron transfer (ET) processes was investigated, giving rise to the celebrated nonadiabatic ET rate formula. In this work, on the basis of the thermodynamic solvation potentials analysis, we reexamine Marcus’ formula with respect to the Rice-Ramsperger-Kassel-Marcus (RRKM) theory. Interestingly, the obtained RRKM analogue, which recovers the original Marcus’ rate that is in a linear solvation scenario, is also applicable to the nonlinear solvation scenarios, where the multiple curve-crossing of solvation potentials exists. Parallelly, we revisit the corresponding Fermi’s golden rule results, with some critical comments against the RRKM analogue proposed in this work. For illustration, we consider the quadratic solvation scenarios, on the basis of physically well-supported descriptors.

     

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    通讯作者: 陈斌, bchen63@163.com
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      沈阳化工大学材料科学与工程学院 沈阳 110142

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