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In the pioneering work by R. A. Marcus, the solvation effect on electrontransfer (ET) processes was investigated, giving rise to the celebratednonadiabatic ET rate formula. In this work, on the basis of the thermodynamicsolvation potentials analysis, we reexamine Marcus' formula with respect to theRice-Ramsperger-Kassel-Marcus (RRKM) theory. Interestingly, the obtained RRKManalogue, which recovers the original Marcus' rate that is in a linearsolvation 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 criticalcomments against the RRKM analogue proposed in this work. For illustration, weconsider the quadratic solvation scenarios, on the basis of physicallywell-supported descriptors.

chinese journal of chemical physics/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