Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System.
Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System.
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DOI：
10.1021/acs.jpca.7b04344
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发表时间：
2017-09-21
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;Kellis DL;Patten LK;Davis PH;Lee J;Graugnard E;Yurke B;Knowlton WB
染料聚集体中的相干激子离域引起了各种有趣的光学现象，包括J-和h -聚集体行为和Davydov分裂。在室温下表现出相干激子离域的系统对人工光收集装置、比色检测方案和量子计算机的发展很感兴趣。在这里，我们报告了一个简单的染料系统模板的DNA，表现出可调的光学性质。在低盐和DNA浓度下，具有两种内部功能化Cy5染料的DNA双工（即二聚体）持续存在，并表现出主要的j聚集行为。增加盐和/或DNA浓度被发现可以通过分支迁移促进两个DNA双链之间的偶联，从而形成具有h聚集行为的四臂结（即四聚体）。这种h -四聚体聚集体在其吸光度光谱中表现出惊人的大Davydov分裂，使溶液的颜色从青色变为紫色，并提供了相干激子离域的明确证据。
Coherent exciton delocalization in dye aggregate systems gives rise to a variety of intriguing optical phenomena, including J- and H-aggregate behavior and Davydov splitting. Systems that exhibit coherent exciton delocalization at room temperature are of interest for the development of artificial light-harvesting devices, colorimetric detection schemes, and quantum computers. Here, we report on a simple dye system templated by DNA that exhibits tunable optical properties. At low salt and DNA concentrations, a DNA duplex with two internally functionalized Cy5 dyes (i.e., dimer) persists and displays predominantly J-aggregate behavior. Increasing the salt and/or DNA concentrations was found to promote coupling between two of the DNA duplexes via branch migration, thus forming a four-armed junction (i.e., tetramer) with H-aggregate behavior. This H-tetramer aggregate exhibits a surprisingly large Davydov splitting in its absorbance spectrum that produces a visible color change of the solution from cyan to violet and gives clear evidence of coherent exciton delocalization.
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影响因子：
2.3
作者：
Eisfeld, A;Briggs, JS
通讯作者：
Briggs, JS
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作者：
BONIFACIO, R;LUGIATO, LA
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LUGIATO, LA
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作者：
DUCKETT, DR;MURCHIE, AIH;LILLEY, DMJ
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作者：
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通讯作者：
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15
作者：
Asanuma, H;Shirasuka, K;Komiyama, M
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