Excitonic coupling in linear and trefoil trimer perylenediimide molecules probed by single-molecule spectroscopy.
Excitonic coupling in linear and trefoil trimer perylenediimide molecules probed by single-molecule spectroscopy.
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通过单分子光谱探测线性和三叶形三聚体苝二酰亚胺分子中的激子耦合。
DOI：
10.1021/jp307394x
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发表时间：
2012
期刊：
影响因子：
--
通讯作者：
Dongho Kim
中科院分区：
文献类型：
--
作者：
Hyejin Yoo;Shu Furumaki;Jaesung Yang;Jieun Lee;Heejae Chung;Tatsuya Oba;H. Kobayashi;B. Rybtchinski;Thea M. Wilson;M. Wasielewski;M. Vacha;Dongho Kim
苝二酰亚胺 (PDI) 分子是多发色团阵列内电子相互作用光物理研究的有希望的构建模块。这种PDI阵列是制造有机发光二极管、有机半导体和生物传感器等分子纳米器件的重要材料，因为它们具有高光稳定性、化学和物理惰性、电子亲和力以及在整个可见光谱范围内的高着色强度。在这项工作中，PDI 被组织成线性 (L3) 和三叶形 (T3) 三聚体分子，并通过单分子荧光显微镜进行研究，以探讨分子结构与发色团间电子相互作用之间的关系。我们通过监测每个组成发色团的顺序光漂白后单分子荧光光谱中的光谱峰位移，发现 L3 和 T3 中的耦合强度分布广泛，因此 PDI 单元之间存在强/弱耦合。此外，我们使用宽视场散焦成像技术来解决嵌入 PMMA 聚合物基质中的 L3 和 T3 分子结构的异质性。通过对两组实验结果进行系统比较，我们可以推断出分子间相互作用与分子结构之间的相关性。我们的结果表明使用合适的多发色团结构可以控制 PDI 分子间相互作用。
Perylenediimide (PDI) molecules are promising building blocks for photophysical studies of electronic interactions within multichromophore arrays. Such PDI arrays are important materials for fabrication of molecular nanodevices such as organic light-emitting diodes, organic semiconductors, and biosensors because of their high photostability, chemical and physical inertness, electron affinity, and high tinctorial strength over the entire visible spectrum. In this work, PDIs have been organized into linear (L3) and trefoil (T3) trimer molecules and investigated by single-molecule fluorescence microscopy to probe the relationship between molecular structures and interchromophoric electronic interactions. We found a broad distribution of coupling strengths in both L3 and T3 and hence strong/weak coupling between PDI units by monitoring spectral peak shifts in single-molecule fluorescence spectra upon sequential photobleaching of each constituent chromophore. In addition, we used a wide-field defocused imaging technique to resolve heterogeneities in molecular structures of L3 and T3 embedded in a PMMA polymer matrix. A systematic comparison between the two sets of experimental results allowed us to infer the correlation between intermolecular interactions and molecular structures. Our results show control of the PDI intermolecular interactions using suitable multichromophoric structures.
影响因子：
15
作者：
Han, Jason J.;Shaller, Andrew D.;Li, Alexander D. Q.
通讯作者：
Li, Alexander D. Q.