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首页> 外文期刊>RSC Advances >Electronic and spatial control over the formation of transient ion pairs during photoinduced electron transfer between proflavine–amine systems in a subpicosecond time regime
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Electronic and spatial control over the formation of transient ion pairs during photoinduced electron transfer between proflavine–amine systems in a subpicosecond time regime

机译：亚皮秒时间范围内前黄酮-胺系统之间光诱导电子转移过程中瞬态离子对形成的电子和空间控制

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Probing photoinduced electron transfer (PET) in solution in terms of rate of reaction and reaction free energy is a great challenge in physical chemistry. Several factors such as solvent polarity, viscosity, and electronic coupling between reacting species control the overall rate of the reaction. However, the unambiguous reaction mechanism is still an important area of research. Earlier, our studies on proflavine–DMA and proflavine–TEA electron donor–acceptor systems revealed the dynamics of the diffusion controlled aspect of PET. Herein, we have extended our investigation in a higher time resolution i.e. in the femtosecond–picosecond timescale to decipher the incidents occurring at the time regime associated with PET. Our present contribution sheds light on the controlling factors of polarity, viscosity, and microheterogeneity, leading to the confinement of reactants at the molecular level. We also tried to qualitatively as well as quantitatively probe these factors. Our present investigation reveals that electron transfer in these two systems is dependent on several factors. In the case of alcoholic solvents, the fastest fluorescence decay components are the result of the formation of a contact ion pair (CIP) as well as direct electron transfer and therefore depend on the dielectric of the medium. On the other hand, in a heterogeneous medium, compartmentalization of reactants and interaction between the components with head groups and tail parts of micelles, depending on the overall charge of a particular micelle, are the controlling factors for the reaction dynamics.
机译：在反应速率和反应自由能方面探测溶液中的光致电子转移（PET）是物理化学中的一大挑战。诸如溶剂极性，粘度和反应物种之间的电子耦合等多种因素控制着反应的总速率。但是，明确的反应机理仍然是重要的研究领域。之前，我们对前黄素-DMA和前黄素-TEA电子供体-受体系统的研究揭示了PET扩散控制方面的动态。在此，我们以飞秒级至皮秒级的时间分辨率更高的时间分辨率即扩展了我们的研究，以破译与PET相关的时间范围内发生的事件。我们目前的贡献揭示了极性，粘度和微异质性的控制因素，从而将反应物限制在分子水平上。我们还尝试定性和定量探查这些因素。我们目前的研究表明，这两个系统中的电子转移取决于几个因素。对于酒精溶剂，最快的荧光衰减成分是接触离子对（CIP）形成以及直接电子转移的结果，因此取决于介质的介电常数。另一方面，在异质介质中，取决于特定胶束的总电荷，反应物的分隔以及胶束的头部和尾部之间的组分之间的相互作用是反应动力学的控制因素。

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