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Narra, Sudhakar; Nishimura, Yoshifumi; Witek, Henryk A.; Shigeto, Shinsuke
Chemphyschem, October 6, 2014, Volume: 15, Issue: 14Journal Article
Back electron transfer (BET) is one of the important processes that govern the decay of generated ion pairs in intermolecular photoinduced electron transfer reactions. Unfortunately, a detailed mechanism of BET reactions remains largely unknown in spite of their importance for the development of molecular photovoltaic structures. Here, we examine the BET reaction of pyrene (Py) and 1,4‐dicyanobenzene (DCB) in acetonitrile (ACN) by using time‐resolved near‐ and mid‐IR spectroscopy. The Py dimer radical cation (Py2.+) and DCB radical anion (DCB.−) generated after photoexcitation of Py show asynchronous decay kinetics. To account for this observation, we propose a reaction mechanism that involves electron transfer from DCB.− to the solvent and charge recombination between the resulting ACN dimer anion and Py2.+. The unique role of ACN as a charge mediator revealed herein could have implications for strategies that retard charge recombination in dye‐sensitized solar cells. Who receives the electron? A thorough kinetic analysis of time‐resolved near‐ and mid‐IR spectra has clarified the mechanism of back electron transfer in the intermolecular photoinduced electron transfer reaction of pyrene and 1,4‐dicyanobenzene in acetonitrile (see figure). We found that acetonitrile plays a key role as a charge mediator between the charge carriers induced after photoexcitation and thus governs the overall charge recombination dynamics.
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