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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Triplet Population Dynamics of Single Conjugated Polymer Molecules and Nanoscale Assemblies
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Triplet Population Dynamics of Single Conjugated Polymer Molecules and Nanoscale Assemblies

机译：单缀合聚合物分子和纳米级组件的三联人口群体动力学

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The formation of long-lived triplet excited electronic states has important ramifications for conjugated organic materials used in optoelectronic devices. In the case of polymers, unravelling various structural factors mediating triplet processes is difficult because of heterogeneity effects due to intrinsic molecular weight polydispersity and large conformational degrees of freedom. Conformation-dependent electronic coupling between chromophore segments also modulates relaxation branching ratios that may vary substantially from molecule to molecule. However, ensemble-level spectroscopy experiments typically average over distinct responses, which disguises important qualities of the overall material photophysical landscape. Suppression of heterogeneity by diluting polymers into inert solid hosts permits single molecule level investigations of conformation-dependent triplet dynamics thereby avoiding the most insidious consequences of ensemble averaging. Interestingly, the multichromophoric nature of polymers can lead to significant likelihoods of multiple coexisting triplets, where population dynamics are revealed from fluorescence quenching dynamics on time scales comparable to triplet lifetimes (i.e., mu s to ms). Stochastic photodynamic models are then used to extract key kinetic constants, including bimolecular triplet-triplet annihilation, that tend to exhibit pronounced dependences on polymer conformational ordering. Furthermore, simple processing strategies to selectively control chain conformation and packing order in hierarchical polymer assemblies can be combined with experiment and modeling to uncover the evolution in triplet processes from single molecule to bulk material levels. We posit that molecular-level control can be harnessed to more accurately manage triplet yields and interactions over a large range of time scales, which has potential uses in multiexciton harvesting schemes, such as singlet fission.
机译：长寿命的三联兴奋电子态的形成具有用于光电器件中使用的共轭有机材料的重要条件。在聚合物的情况下，由于内在分子量多分散性和大构象的自由度，难以揭示介导三重态过程的各种结构因子是困难的。在发色团段之间的构象依赖性电子耦合还调节弛豫支链，其可以基本上从分子到分子的分子变化。然而，集合级光谱实验通常在不同的反应上平均，这伪装了整体材料光物理景观的重要品质。通过将聚合物稀释到惰性固体宿主中抑制异质性允许单一分子水平研究依赖于依赖性三联动态，从而避免了集合平均的最致命化的后果。有趣的是，聚合物的多尺寸性质​​可以导致多个共存三胞胎的显着可能性，其中从荧光猝灭动态揭示了与三重态寿命相当的荧光猝灭动态的群体动力学（即MU S至MS）。然后用于提取随机光动力学模型来提取关键动力学常数，包括双分子三重态 - 三联湮灭，其倾向于表现出对聚合物构象排序的显着依赖性。此外，可以将简单的加工策略选择性地控制分层聚合物组件中的链构象和包装顺序可以与实验和建模结合，以将来自单个分子的三重态过程中的进化涂布为散装材料水平。我们对可以利用的分子水平控制来更准确地管理三联物质产生和在大范围的时间尺度上的相互作用，这在多曲线收集方案中具有潜在的用途，例如单线裂缝。

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