Ultrafast Experiments on the Role of Vibrational Modes in Electron Transfer
MINNESOTA UNIV MINNEAPOLIS DEPT OF CHEMISTRY
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The role of vibrational modes in ultrafast photoinduced intramolecular electron transfer reactions is explored. Femtosecond resolved experiments on two chemical classes will be described, namely, metal-mental intervalence electron transfer in mixed valence compounds and intromolecular charge recombinationseparation in organic dooracceptor compound class, the betaines. The results have been analyzed to reveal the complex interactions of intromolecular and intermolecular modes in electron transfer reactions. The study of charge transfer processes, and in particular homogeneous electron transfer ET in solution, is at the forefront of the study of the molecular details of chemical reactions in liquids. The last decade has brought progress to many central problems in ET research, including the role of the solvent in these reactions, the involvement of vibrational degrees of freedom, the role of nuclear tunnneling of the solvent and solute and related quantum mechanical effects, the pathway and mechanism of electronic interactions, including long range ET, and other aspects of biological and heterogeneous ET. Recent reviews of the foundations of ET theories have been given by Newton and Sutin and Marcus and Sutin. Theories of ET reactions in solution are formulated in terms of a model in which the transferring electron is localized at a donor molecular site in the reactant and at a different acceptor molecular site in the product.
- Physical Chemistry
- Solid State Physics