NDLI: A non-Marcus model for electrostatic fluctuations in long range electron transfer

Content Provider	Springer Nature Link
Author	Fletcher, Stephen
Copyright Year	2007
Abstract	We propose a new model for the elementary act of electron transfer between two species in solution. The central idea is that the solution in the immediate vicinity of each species may be represented by an equivalent circuit consisting of a Debye circuit shunted by a resistor. Based on this insight, we derive a new formula for the one-dimensional potential energy profile of a coupled donor–acceptor pair at finite (but large) separation d, along a charge-fluctuation reaction co-ordinate, at fixed radii of the transition states. The corresponding reorganisation energy of the reaction is also derived, and it is found to differ from that in the Marcus theory. In particular, the new model predicts that the reorganisation energy is independent of the static dielectric constant of the solution, whereas the old model predicts a strong dependence. The difference is traced to the fact that the Marcus theory omits consideration of the work required to form the charge fluctuations and focuses instead on the work required to localise the charge fluctuations. In general, the equivalent circuit approach permits many of the difficult-to-derive equations of non-equilibrium polarisation theory to be written down by inspection.
Starting Page	965
Ending Page	969
Page Count	5
File Format	PDF
ISSN	14328488
Journal	Journal of Solid State Electrochemistry
Volume Number	11
Issue Number	7
e-ISSN	14330768
Language	English
Publisher	Springer-Verlag
Publisher Date	2007-04-18
Publisher Place	Berlin, Heidelberg
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	Marcus theory Electron transfer theory Reorganisation energy Equivalent circuit Electrostatic fluctuations Electronic and Computer Engineering Condensed Matter Characterization and Evaluation of Materials Industrial Chemistry/Chemical Engineering Analytical Chemistry Physical Chemistry
Content Type	Text
Resource Type	Article
Subject	Condensed Matter Physics Materials Science Electrical and Electronic Engineering Electrochemistry

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