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Tunable Electronic Structure via DNA-Templated Heteroaggregates of Two Distinct Cyanine Dyes.
Huff, Jonathan S; Díaz, Sebastián A; Barclay, Matthew S; Chowdhury, Azhad U; Chiriboga, Matthew; Ellis, Gregory A; Mathur, Divita; Patten, Lance K; Roy, Simon K; Sup, Aaron; Biaggne, Austin; Rolczynski, Brian S; Cunningham, Paul D; Li, Lan; Lee, Jeunghoon; Davis, Paul H; Yurke, Bernard; Knowlton, William B; Medintz, Igor L; Turner, Daniel B; Melinger, Joseph S; Pensack, Ryan D.
Affiliation
  • Huff JS; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Díaz SA; Center for Bio/Molecular Science and Engineering Code 6900, Electronics Science and Technology Division Code 6800, U.S. Naval Research Laboratory, Washington, District of Columbia 20375, United States.
  • Barclay MS; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Chowdhury AU; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Chiriboga M; Center for Bio/Molecular Science and Engineering Code 6900, Electronics Science and Technology Division Code 6800, U.S. Naval Research Laboratory, Washington, District of Columbia 20375, United States.
  • Ellis GA; Volgenau School of Engineering, George Mason University, Fairfax, Virginia 22030, United States.
  • Mathur D; Center for Bio/Molecular Science and Engineering Code 6900, Electronics Science and Technology Division Code 6800, U.S. Naval Research Laboratory, Washington, District of Columbia 20375, United States.
  • Patten LK; Center for Bio/Molecular Science and Engineering Code 6900, Electronics Science and Technology Division Code 6800, U.S. Naval Research Laboratory, Washington, District of Columbia 20375, United States.
  • Roy SK; College of Science, George Mason University, Fairfax, Virginia 22030, United States.
  • Sup A; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Biaggne A; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Rolczynski BS; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Cunningham PD; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Li L; Center for Bio/Molecular Science and Engineering Code 6900, Electronics Science and Technology Division Code 6800, U.S. Naval Research Laboratory, Washington, District of Columbia 20375, United States.
  • Lee J; Center for Bio/Molecular Science and Engineering Code 6900, Electronics Science and Technology Division Code 6800, U.S. Naval Research Laboratory, Washington, District of Columbia 20375, United States.
  • Davis PH; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Yurke B; Center for Advanced Energy Studies, Idaho Falls, Idaho 83401, United States.
  • Knowlton WB; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Medintz IL; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Turner DB; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
  • Melinger JS; Center for Advanced Energy Studies, Idaho Falls, Idaho 83401, United States.
  • Pensack RD; Micron School of Materials Science & Engineering, Department of Physics, Department of Chemistry & Biochemistry, Department of Electrical & Computer Engineering, Boise State University, Boise, Idaho 83725, United States.
J Phys Chem C Nanomater Interfaces ; 126(40): 17164-17175, 2022 Oct 13.
Article in En | MEDLINE | ID: mdl-36268205
ABSTRACT
Molecular excitons are useful for applications in light harvesting, organic optoelectronics, and nanoscale computing. Electronic energy transfer (EET) is a process central to the function of devices based on molecular excitons. Achieving EET with a high quantum efficiency is a common obstacle to excitonic devices, often owing to the lack of donor and acceptor molecules that exhibit favorable spectral overlap. EET quantum efficiencies may be substantially improved through the use of heteroaggregates-aggregates of chemically distinct dyes-rather than individual dyes as energy relay units. However, controlling the assembly of heteroaggregates remains a significant challenge. Here, we use DNA Holliday junctions to assemble homo- and heterotetramer aggregates of the prototypical cyanine dyes Cy5 and Cy5.5. In addition to permitting control over the number of dyes within an aggregate, DNA-templated assembly confers control over aggregate composition, i.e., the ratio of constituent Cy5 and Cy5.5 dyes. By varying the ratio of Cy5 and Cy5.5, we show that the most intense absorption feature of the resulting tetramer can be shifted in energy over a range of almost 200 meV (1600 cm-1). All tetramers pack in the form of H-aggregates and exhibit quenched emission and drastically reduced excited-state lifetimes compared to the monomeric dyes. We apply a purely electronic exciton theory model to describe the observed progression of the absorption spectra. This model agrees with both the measured data and a more sophisticated vibronic model of the absorption and circular dichroism spectra, indicating that Cy5 and Cy5.5 heteroaggregates are largely described by molecular exciton theory. Finally, we extend the purely electronic exciton model to describe an idealized J-aggregate based on Förster resonance energy transfer (FRET) and discuss the potential advantages of such a device over traditional FRET relays.

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Phys Chem C Nanomater Interfaces Year: 2022 Document type: Article Affiliation country: United States

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Phys Chem C Nanomater Interfaces Year: 2022 Document type: Article Affiliation country: United States
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