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A multitude of approaches addressing the diffusion influence of distance electron-transfer phenomena has been suggested. We employ the DET framework here, as it has proven valuable in a variety of related studies. However, we do not imply that DET is the only model able to comprehensively account for the experimental data. the inclined reader should realize that DET and the approach paved by Tachiya and Fayer are equivalent, with one resulting from the other by adjoining the differential operator of the diffusion equation. the mathematical tools necessary to prove the equivalence of these and related Sturm-Liouville problems are, for example, summarized in Mathematics for Physicists (Eds.: P. Dennery, A. Krzywicki), Dover, New York
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note
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Note, however, that a priori differential encounter theory does not require a strict distinction of the SIP or TIP, the transition being (possibly) smooth. Indeed, the TIP could, in the DET picture, be introduced either as an "efficiently coupled" ion pair or as an additional contact species. Literature suggests the second proposition, which is also assumed here. It is crucial to note that a TIP-free model is sufficient for modeling the diffusive ET deactivation at low to moderate concentrations in most cases. This statement also applies to the interpretation of the Rehm-Weiler experiment given in ref. [22]. Apparently, the effective reaction volume associated with the TIP is too small to contribute significantly, except possibly at exceptionally large concentrations. It is expected that the recent advancement in spectroscopic techniques will stimulate research on the bending questions of the TIP. Our study makes it clear that no correct interpretation of these experiments will be possible without due consideration of the solvent structure.
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