Photoinduced mechanisms for energy conversion must efficiently convert transient photoexcitations into long-lived states capable of storing energy for future use. Photochemical approaches have garnered much attention as a complement to photovoltaic energy conversion platforms. Molecular design of photoactive molecules should incorporate the effects of their environment on their photophysical behavior, the creation of intermediate states, and on their subsequent chemical transformations. We use the photolysis of bimolecular charge transfer complexes in solution to generate reactive radical ions in their solvent-equilibrated electronic ground state. In polar protic media, these photoexcitations undergo efficient, ultrafast dissociation to ion pairs and equilibrate with their solvent environment before the resulting radical ions engage in electron transfer and proton abstraction on subnanosecond time scales. The local environment of photogenerated radical ions can be designed to promote solvent–solute interactions that tune their reaction pathways.<br/>

Role of polar protic solvents in the dissociation and reactivity of photogenerated radical ion pairs

ACS Fall 2020 Virtual Meeting

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