Ying Chen, Rui-xue Xu, Hong-wei Ke, Yi-jing Yan. Electron Transfer Theory Revisit: Motional Narrowing Induced Non-Markovian Rate Processes[J]. Chinese Journal of Chemical Physics , 2007, 20(4): 438-444. doi: 10.1088/1674-0068/20/04/438-444
Citation: Ying Chen, Rui-xue Xu, Hong-wei Ke, Yi-jing Yan. Electron Transfer Theory Revisit: Motional Narrowing Induced Non-Markovian Rate Processes[J]. Chinese Journal of Chemical Physics , 2007, 20(4): 438-444. doi: 10.1088/1674-0068/20/04/438-444

Electron Transfer Theory Revisit: Motional Narrowing Induced Non-Markovian Rate Processes

doi: 10.1088/1674-0068/20/04/438-444
Funds:  This work was supported from the RGC Hong Kong(No.604006), the National Natural Science Foundationof China (No.50121202), and National Basic ResearchProgram of China (No.2006CB922004). Rui-xue Xuwould also like to thank the support from the NationalN
  • Received Date: 2007-05-21
  • Rev Recd Date: 2007-07-04
  • While the exact theory of chemical reaction rate processes is always non-Markovian, experimental rates do often show practically Markovian that supports kinetics rate constant description. In this work, we propose to use the Kubo's motional narrowing line shape function to characterize the Markovian character of the simplest two-state electron transfer reaction system. On the basis of analytical results, we demonstrate the related Markovianicity parameter as an interplay between the °uctuating solvent environment and the coherent transfer coupling. It is found that a non-Markovian rate process is most likely to occur in a symmetric system in the fast solvent modulation regime, where the resonant tunneling enhancement plays the important role. The e?ect of quantum solvation on electron transfer, which is dominant in the fast modulation regime, will also be highlighted.
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Electron Transfer Theory Revisit: Motional Narrowing Induced Non-Markovian Rate Processes

doi: 10.1088/1674-0068/20/04/438-444
Funds:  This work was supported from the RGC Hong Kong(No.604006), the National Natural Science Foundationof China (No.50121202), and National Basic ResearchProgram of China (No.2006CB922004). Rui-xue Xuwould also like to thank the support from the NationalN

Abstract: While the exact theory of chemical reaction rate processes is always non-Markovian, experimental rates do often show practically Markovian that supports kinetics rate constant description. In this work, we propose to use the Kubo's motional narrowing line shape function to characterize the Markovian character of the simplest two-state electron transfer reaction system. On the basis of analytical results, we demonstrate the related Markovianicity parameter as an interplay between the °uctuating solvent environment and the coherent transfer coupling. It is found that a non-Markovian rate process is most likely to occur in a symmetric system in the fast solvent modulation regime, where the resonant tunneling enhancement plays the important role. The e?ect of quantum solvation on electron transfer, which is dominant in the fast modulation regime, will also be highlighted.

Ying Chen, Rui-xue Xu, Hong-wei Ke, Yi-jing Yan. Electron Transfer Theory Revisit: Motional Narrowing Induced Non-Markovian Rate Processes[J]. Chinese Journal of Chemical Physics , 2007, 20(4): 438-444. doi: 10.1088/1674-0068/20/04/438-444
Citation: Ying Chen, Rui-xue Xu, Hong-wei Ke, Yi-jing Yan. Electron Transfer Theory Revisit: Motional Narrowing Induced Non-Markovian Rate Processes[J]. Chinese Journal of Chemical Physics , 2007, 20(4): 438-444. doi: 10.1088/1674-0068/20/04/438-444

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