Abstract
In 1960 Marcus predicted that rate constants for electron transfer should decrease with -{Delta}G in the inverted region. In the inverted region, -{Delta}G > {lambda}, where {lambda} is the reorganization energy and {Delta}G the free energy loss associated with the electron transfer. Experimental verification of this prediction has been difficult to obtain but has been found by pulse radiolysis in rigid organic glasses, by Closs, Miller, and co-workers in unsymmetrical, linked organics, in accounting for separation yields in photoinduced electron transfer, and by light-induced electron transfer in linked porphyrin-quinone systems. The authors report here the first examples based on transition-metal complexes and, as predicted theoretically, that there is a clear relationship between electron transfer in the inverted region and nonradiative decay in a closely related family of excited states.
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