4.6 Article

Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System

Journal

JOURNAL OF PHYSICAL CHEMISTRY A
Volume 121, Issue 37, Pages 6905-6916

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.7b04344

Keywords

-

Funding

  1. Boise State University Division of Research and Economic Development, NASA Idaho Space Grant Consortium (ISGC)
  2. National Science Foundation INSPIRE [1648655]
  3. Institutional Development Awards (IDeA) from the National Institute of General Medical Sciences [P20GM103408]
  4. National Institutes of Health [P20GM109095]
  5. National Science Foundation [0619793, 0923535]
  6. MJ Murdock Charitable Trust
  7. Idaho State Board of Education
  8. Micron Technology MSE Ph.D. Fellowship
  9. NIGMS [P41-GM103311]
  10. Directorate For Engineering
  11. Div Of Electrical, Commun & Cyber Sys [1648655] Funding Source: National Science Foundation

Ask authors/readers for more resources

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.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.6
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

No Data Available
No Data Available