Large Davydov Splitting and Strong Fluorescence Suppression: An Investigation of Exciton Delocalization in DNA-Templated Holliday Junction Dye Aggregates.
Large Davydov Splitting and Strong Fluorescence Suppression: An Investigation of Exciton Delocalization in DNA-Templated Holliday Junction Dye Aggregates.
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DOI：
10.1021/acs.jpca.7b12668
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发表时间：
2018-03-01
期刊：
影响因子：
--
通讯作者：
Knowlton WB
中科院分区：
文献类型：
--
作者：
Cannon BL;Patten LK;Kellis DL;Davis PH;Lee J;Graugnard E;Yurke B;Knowlton WB
染料聚集体体系中的激子离域是一种通过光谱特征，如Davydov分裂，J-和H-聚集体行为和荧光抑制来揭示的现象。使用DNA作为结构模板来标记染料聚集体使得能够特异性控制聚集体尺寸和染料类型，染料在聚集体内的近端和精确定位，以及用于构建大的模块化二维和三维阵列的方法。在这里，我们报告的染料聚集体，通过一个固定的霍利迪结DNA模板，表现出大的Davydov分裂的吸收光谱（125 nm，397.5 meV），J-和H-聚集体的行为，和几乎完全抑制的荧光发射（~97.6%的抑制）。由于聚集体的独特光学性质，我们已经证明，我们的染料聚集体系统是一个可行的候选人作为一个敏感的吸光度和荧光光学报告。表现出激子离域的DNA模板聚集体可以在光学检测和成像、光捕获、光化学、光学信息处理和量子计算中找到应用。
Exciton delocalization in dye aggregate systems is a phenomenon that is revealed by spectral features, such as Davydov splitting, J- and H-aggregate behavior, and fluorescence suppression. Using DNA as an architectural template to assembledye aggregates enables specific control of the aggregate size and dye type, proximal and precise positioning of the dyes within the aggregates, and a method for constructing large, modular two and three-dimensional arrays. Here, we report on dye aggregates,organized via an immobile Holliday junction DNA template, that exhibit large Davydov splitting of the absorbance spectrum (125nm, 397.5 meV), J- and H-aggregate behavior, and near-complete suppression of the fluorescence emission (~97.6% suppression). Because of the unique optical properties of the aggregates, we have demonstrated that our dye aggregate system is a viable candidate as a sensitive absorbance and fluorescence optical reporter. DNA-templated aggregates exhibiting exciton delocalization may find application in optical detection and imaging, light-harvesting, photovoltaics, optical information processing, and quantum computing.
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