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The Rehm-Weller experiment in view of distant electron transfer
A Rosspeintner1, D R Kattnig, G Angulo
1Graz University of Technology, Technikerstrasse 4/I, 8010 Graz, Austria.
Chemistry (Weinheim an Der Bergstrasse, Germany)
|May 29, 2008
Summary
This study revisits the Rehm-Weller experiment, analyzing the diffusional plateau in electron transfer reactions. Findings reveal this plateau highlights the inherent distance dependence of electron transfer in solution.
Area of Science:
- Photochemistry
- Physical Chemistry
- Electron Transfer Reactions
Background:
- The Rehm-Weller experiment investigates bimolecular fluorescence quenching via electron transfer.
- Long-standing questions persist regarding the features of this electron transfer process, specifically the existence of a diffusional plateau.
Purpose of the Study:
- To analyze the presence and significance of a diffusional plateau in the Rehm-Weller experiment.
- To model the driving-force dependence of electron transfer quenching.
Main Methods:
- Compilation of new experimental quenching rates for a specific electron donor and eighteen electron acceptors in acetonitrile.
- Analysis using differential encounter theory and an extended Marcus theory for the intrinsic electron-transfer step.
Main Results:
- Experimental data are well-modeled only when hydrodynamic effects and solvent structure are included.
- The diffusional control region, or plateau, demonstrates the intrinsic distance dependence of the reaction.
Conclusions:
- The diffusional plateau is a key feature of electron transfer reactions in solution.
- This distance dependence is a general characteristic of electron transfer processes.
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