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Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2017-09-06 00:00:00 , DOI: 10.1021/acs.jpca.7b04344 Brittany L. Cannon 1 , Donald L. Kellis 1 , Lance K. Patten 1 , Paul H. Davis 1 , Jeunghoon Lee 1 , Elton Graugnard 1 , Bernard Yurke 1 , William B. Knowlton 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2017-09-06 00:00:00 , DOI: 10.1021/acs.jpca.7b04344 Brittany L. Cannon 1 , Donald L. Kellis 1 , Lance K. Patten 1 , Paul H. Davis 1 , Jeunghoon Lee 1 , Elton Graugnard 1 , Bernard Yurke 1 , William B. Knowlton 1
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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.
中文翻译：
两国DNA模板染料聚集系统中的相干激子离域。
染料聚集体系统中相干激子的离域化引起了许多有趣的光学现象，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于开发人造光收集设备，比色检测方案和量子计算机很感兴趣。在这里，我们报告由DNA模板化的简单染料系统，该染料系统显示出可调的光学特性。在低盐和DNA浓度下，带有两种内部功能化Cy5染料（即二聚体）的DNA双链体仍然存在，并且主要表现为J聚集行为。发现增加盐和/或DNA浓度可通过分支迁移促进两个DNA双链体之间的偶联，从而形成具有H-聚集行为的四臂连接（即，四聚体）。
更新日期：2017-09-07
中文翻译：
两国DNA模板染料聚集系统中的相干激子离域。
染料聚集体系统中相干激子的离域化引起了许多有趣的光学现象，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于开发人造光收集设备，比色检测方案和量子计算机很感兴趣。在这里，我们报告由DNA模板化的简单染料系统，该染料系统显示出可调的光学特性。在低盐和DNA浓度下，带有两种内部功能化Cy5染料（即二聚体）的DNA双链体仍然存在，并且主要表现为J聚集行为。发现增加盐和/或DNA浓度可通过分支迁移促进两个DNA双链体之间的偶联，从而形成具有H-聚集行为的四臂连接（即，四聚体）。
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