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.

doi:10.1021/acs.jpcc.2c04336

Title: Tunable Electronic Structure via DNA-Templated Heteroaggregates of Two Distinct Cyanine Dyes

Journal Article · Wed Sep 28 00:00:00 EDT 2022 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.2c04336· OSTI ID:1890236

;

; Barclay, Matthew S.; Chowdhury, Azhad U.; Chiriboga, Matthew ^[1]; Ellis, Gregory A.;

^[2];

;

; Sup, Aaron; Biaggne, Austin;

;

; Li, Lan ^[3];

;

^[3];

;

Volgenau School of Engineering, George Mason University, Fairfax, Virginia 22030, United States
College of Science, George Mason University, Fairfax, Virginia 22030, United States
Center for Advanced Energy Studies, Idaho Falls, Idaho 83401, United States

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 hetero-tetramer 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 (1,600 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.

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Research Organization:: Boise State Univ., ID (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: SC0020089

OSTI ID:: 1890236

Alternate ID(s):: OSTI ID: 1890491; OSTI ID: 1892492

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Vol. 126 Journal Issue: 40; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
Molecular excitons
electronic energy transfer
cyanine dye Cy5 and Cy5.5 heteroaggregates
H- and J-aggregates
Förster resonance energy transfer
molecular excitons
absorption
dyes and pigments
electrical energy
fluorescense resonance energy transfer
monomers

Title: Tunable Electronic Structure via DNA-Templated Heteroaggregates of Two Distinct Cyanine Dyes

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