Exciton Delocalization in Indolenine Squaraine Aggregates Templated by DNA Holliday Junction Scaffolds
Abstract
Exciton delocalization plays a prominent role in the photophysics of molecular aggregates, ultimately governing their particular function or application. DNA is a compelling scaffold in which to template molecular aggregates and promote exciton delocalization. As individual dye molecules are the basis of exciton delocalization in molecular aggregates, their judicious selection is important. Motivated by their excellent photostability and spectral properties, here we examine the ability of squaraine dyes to undergo exciton delocalization when aggregated via a DNA Holliday junction (HJ) template. A commercially available indolenine squaraine dye was chosen for the study given its strong structural resemblance to Cy5, a commercially available cyanine dye previously shown to undergo exciton delocalization in DNA HJs. Three types of DNA-dye aggregate configurations—transverse dimer, adjacent dimer, and tetramer—were investigated. Signatures of exciton delocalization were observed in all squaraine-DNA aggregates. Specifically, strong blue shift and Davydov splitting were observed in steady-state absorption spectroscopy and exciton-induced features were evident in circular dichroism spectroscopy. Strongly suppressed fluorescence emission provided additional, indirect evidence for exciton delocalization in the DNA-templated squaraine dye aggregates. To quantitatively evaluate and directly compare the excitonic Coulombic coupling responsible for exciton delocalization, the strength of excitonic hopping interactions between the dyes were obtained bymore »
- Authors:
-
- Boise State Univ., ID (United States)
- SETA BioMedicals, LLC, Urbana, IL (United States)
- Publication Date:
- Research Org.:
- Boise State Univ., ID (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Science Foundation (NSF); National Institute of General Medical Sciences (NIGMS); National Institutes of Health (NIH); MJ Murdock Charitable Trust; Idaho State Board of Education
- OSTI Identifier:
- 1670511
- Grant/Contract Number:
- SC0020089; 1648655; P20GM103408; P20GM109095; 0619793; 0923535
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 43; Related Information: SUPPORTING INFORMATION Exciton Delocalization in Indolenine Squaraine Aggregates Templated byDNA Holliday Junction Scaffolds1Olga A. Mass; 1Christopher K. Wilson; 1Simon K. Roy; Matthew S. Barclay; 1Lance K. Patten;2Ewald A. Terpetschnig; *1,3Jeunghoon Lee; *1Ryan D. Pensack; *1,4Bernard Yurke;*1,4William B. Knowlton.1Micron School of Materials Science & Engineering, 3Department of Chemistry andBiochemistry, 4Department of Electrical & Computer Engineering, Boise State University, Boise,Idaho 83725, United States2SETA BioMedicals, LLC, 2014 Silver Court East, Urbana, IL 61801, United States; Journal ID: ISSN 1520-6106
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Exciton delocalization; Indolenine Squaraine dye-DNA aggregates; DNA Holliday junctions; Davydov splitting; H-type packing Scaffolds
Citation Formats
Mass, Olga A., Wilson, Christopher Kimo, Roy, Simon K., Barclay, Matthew S., Patten, Lance K., Terpetschnig, Ewald A., Lee, Jeunghoon, Pensack, Ryan D., Yurke, Bernard, and Knowlton, William B.. Exciton Delocalization in Indolenine Squaraine Aggregates Templated by DNA Holliday Junction Scaffolds. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcb.0c06480.
Mass, Olga A., Wilson, Christopher Kimo, Roy, Simon K., Barclay, Matthew S., Patten, Lance K., Terpetschnig, Ewald A., Lee, Jeunghoon, Pensack, Ryan D., Yurke, Bernard, & Knowlton, William B.. Exciton Delocalization in Indolenine Squaraine Aggregates Templated by DNA Holliday Junction Scaffolds. United States. https://doi.org/10.1021/acs.jpcb.0c06480
Mass, Olga A., Wilson, Christopher Kimo, Roy, Simon K., Barclay, Matthew S., Patten, Lance K., Terpetschnig, Ewald A., Lee, Jeunghoon, Pensack, Ryan D., Yurke, Bernard, and Knowlton, William B.. Wed .
"Exciton Delocalization in Indolenine Squaraine Aggregates Templated by DNA Holliday Junction Scaffolds". United States. https://doi.org/10.1021/acs.jpcb.0c06480. https://www.osti.gov/servlets/purl/1670511.
@article{osti_1670511,
title = {Exciton Delocalization in Indolenine Squaraine Aggregates Templated by DNA Holliday Junction Scaffolds},
author = {Mass, Olga A. and Wilson, Christopher Kimo and Roy, Simon K. and Barclay, Matthew S. and Patten, Lance K. and Terpetschnig, Ewald A. and Lee, Jeunghoon and Pensack, Ryan D. and Yurke, Bernard and Knowlton, William B.},
abstractNote = {Exciton delocalization plays a prominent role in the photophysics of molecular aggregates, ultimately governing their particular function or application. DNA is a compelling scaffold in which to template molecular aggregates and promote exciton delocalization. As individual dye molecules are the basis of exciton delocalization in molecular aggregates, their judicious selection is important. Motivated by their excellent photostability and spectral properties, here we examine the ability of squaraine dyes to undergo exciton delocalization when aggregated via a DNA Holliday junction (HJ) template. A commercially available indolenine squaraine dye was chosen for the study given its strong structural resemblance to Cy5, a commercially available cyanine dye previously shown to undergo exciton delocalization in DNA HJs. Three types of DNA-dye aggregate configurations—transverse dimer, adjacent dimer, and tetramer—were investigated. Signatures of exciton delocalization were observed in all squaraine-DNA aggregates. Specifically, strong blue shift and Davydov splitting were observed in steady-state absorption spectroscopy and exciton-induced features were evident in circular dichroism spectroscopy. Strongly suppressed fluorescence emission provided additional, indirect evidence for exciton delocalization in the DNA-templated squaraine dye aggregates. To quantitatively evaluate and directly compare the excitonic Coulombic coupling responsible for exciton delocalization, the strength of excitonic hopping interactions between the dyes were obtained by simultaneous fitting the experimental steady-state absorption and CD spectra via a Holstein-like Hamiltonian in which, following the theoretical approach of Kühn, Renger, and May, the dominant vibrational mode is explicitly considered. The excitonic hopping strength within indolenine squaraines was found to be comparable to that of the analogous Cy5 DNA-templated aggregate. The squaraine aggregates adopted primarily an H-type (dyes oriented parallel to each other) spatial arrangement. Extracted geometric details of dye mutual orientation in the aggregates enabled close comparison of aggregate configurations and the elucidation of the influence of dye angular relationship on excitonic hopping interactions in squaraine aggregates. Furthermore, these results encourage the application of squaraine-based aggregates in next generation systems driven by molecular excitons.},
doi = {10.1021/acs.jpcb.0c06480},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 43,
volume = 124,
place = {United States},
year = {2020},
month = {10}
}
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Exciton Transport in Molecular Aggregates - From Natural Antennas to Synthetic Chromophore Systems
journal, July 2017
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Stark Spectroscopy of Size-Selected Helical H-Aggregates of a Cyanine Dye Templated by Duplex DNA. Effect of Exciton Coupling on Electronic Polarizabilities †
journal, May 2003
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Analysis of the UV/Vis and CD Spectral Line Shapes of Carotenoid Assemblies: Spectral Signatures of Chiral H -Aggregates
journal, April 2009
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Determining the spatial coherence of excitons from the photoluminescence spectrum in charge-transfer J-aggregates
journal, December 2016
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Molecular, Nematic and Crystal States of I: I-Diethyl--Cyanine Chloride
journal, April 1937
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