Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 121, Issue 37, Pages 6905-6916Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.7b04344
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Funding
- Boise State University Division of Research and Economic Development, NASA Idaho Space Grant Consortium (ISGC)
- National Science Foundation INSPIRE [1648655]
- Institutional Development Awards (IDeA) from the National Institute of General Medical Sciences [P20GM103408]
- National Institutes of Health [P20GM109095]
- National Science Foundation [0619793, 0923535]
- MJ Murdock Charitable Trust
- Idaho State Board of Education
- Micron Technology MSE Ph.D. Fellowship
- NIGMS [P41-GM103311]
- Directorate For Engineering
- Div Of Electrical, Commun & Cyber Sys [1648655] Funding Source: National Science Foundation
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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.
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