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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System
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Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System

机译:两种DNA模板染料综合体系中的相干激子临床化

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src="http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpcafh/2017/jpcafh.2017.121.issue-37/acs.jpca.7b04344/20170915/images/medium/jp-2017-04344y_0007.gif">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.
机译:src =“http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jpcafh/2017/jpcafh.2017.121.issue-37/acs.jpca.7b04344/20170915/images/medium /jp-2017-04344Y_0007.gif“染料骨料系统中的”膨干激子临床化产生了各种有趣的光学现象,包括J-和H-骨料行为和Davydov分裂。在室温下表现出相干激子删除化的系统对于人工光收集装置,比色检测方案和量子计算机的开发感兴趣。在这里,我们报告了DNA模板的简单染料系统,其具有可调谐光学性质。在低盐和DNA浓度下,具有两个内官能化Cy5染料(即二聚体)的DNA双链体持续并显示主要是J-骨料行为。发现盐和/或DNA浓度增加通过分支迁移促进两​​种DNA双链体之间的偶联,从而形成具有H-聚集行为的四臂结(即,四聚体)。该H-四聚体聚集体在其吸光度谱中展示了一个令人惊讶的大型达维Davydov分裂,其从青色从青色溶液到紫色产生了可见的颜色变化,并提供了连贯的激子删除的明确证据。

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    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

    Micron School of Materials Science &

    Engineering Department of Chemistry &

    Biochemistry and Department of Electrical &

    Computer Engineering Boise State University Boise Idaho 83725 United States;

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  • 正文语种 eng
  • 中图分类 物理化学(理论化学)、化学物理学;
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