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• W2080761013 abstract "The mechanistic conundrum is commonly posed by the intrinsic structural disconnect between a bimolecular (reactive) intermediate that is fleetingly detected spectroscopically in solution versus that rigorously defined by isolation and X-ray crystallography. We resolve this ambiguity by the combined experimental and theoretical application of the solvent media probe to the transient (1:1) precursor complex in the simplest chemical reaction involving direct adiabatic electron transfer (ET) among various donor/acceptor pairs. Of particular help in our resolution of such an important ET problem is the characterization of the bimolecular precursor complex as Robin−Day class II (localized) or class III (delocalized) from either the solvent-dependent or the solvent-independent response of the diagnostic intervalence absorption bands for the quantitative evaluation of the electronic coupling elements. The magnitudes of these intracomplex bindings are confirmed by theoretical (ab initio and DFT) computations that derive from X-ray structures and Marcus−Hush theories. Most importantly, the experimental solvent-induced ET barriers evaluated from the intervalence absorption bands are also quantitatively verified by the calculated outer-shell reorganization energies to establish unambiguously the intimate interconnection between the loosely bound bimolecular intermediate identified concurrently in solution and in the solid state." @default.
• W2080761013 created "2016-06-24" @default.
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• W2080761013 date "2008-01-23" @default.
• W2080761013 modified "2023-10-16" @default.
• W2080761013 title "The Spectral Elucidation versus the X-ray Structure of the Critical Precursor Complex in Bimolecular Electron Transfers: Application of Experimental/Theoretical Solvent Probes to Ion-Radical (Redox) Dyads" @default.
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• W2080761013 doi "https://doi.org/10.1021/ja076591b" @default.
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