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Article
Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System
The Journal of Physcial Chemistry A
  • Brittany L. Cannon, Boise State University
  • Donald L. Kellis, Boise State University
  • Lance K. Patten, Boise State University
  • Paul H. Davis, Boise State University
  • Jeunghoon Lee, Boise State University
  • Elton Graugnard, Boise State University
  • Bernard Yurke, Boise State University
  • William B. Knowlton, Boise State University
Document Type
Article
Publication Date
9-21-2017
DOI
http://dx.doi.org/10.1021/acs.jpca.7b04344
Disciplines
Abstract

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.

Citation Information
Brittany L. Cannon, Donald L. Kellis, Lance K. Patten, Paul H. Davis, et al.. "Coherent Exciton Delocalization in a Two-State DNA-Templated Dye Aggregate System" The Journal of Physcial Chemistry A (2017)
Available at: http://works.bepress.com/elton_graugnard/67/