skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

This content will become publicly available on April 15, 2020

Title: Directed Energy Transfer through DNA-templated J-aggregates

Abstract

Strongly coupled molecular dye aggregates have unique optoelectronic properties that often resemble those of light harvesting complexes found in nature. The exciton dynamics in coupled dye aggregates could enhance the long-range transfer of optical excitation energy with high efficiency. In principle, dye aggregates could serve as important components in molecular-scale photonic devices, however, rational design of these coupled dye aggregates with precise control over their organization, interactions and dynamics remains a challenge. DNA nanotechnology has recently been used to build an excitonic circuit by organizing pseudoisocyanine (PIC) dyes forming J-aggregates on the templates of poly(dA)-poly(dT) DNA duplexes. Here, the excitonic properties of the PIC J-aggregates on DNA are characterized spectroscopically in detail using poly(dA)-poly(dT) tract lengths of 24 and 48 base pairs. The excitonic properties of these DNA templated dye assemblies depend on the length and sequence of the DNA template. The incorporation of a gap of two GC base pairs between two segments of poly(dA)-poly(dT) DNA markedly reduces the delocalization of excitation in the J-aggregates.Using a quantum dot (QD) as the light absorber and energy donor and using Alexa Fluor 647 (AF647) as the energy acceptor, with a DNA-templated J-aggregate in between, significant energy transfer from QD to AF647more » is observed over a distance far longer than possible without the aggregate bridge. By comparing the efficiency of energy transfer through a continuous J-aggregate with the efficiency when the aggregate has a discontinuity in the middle, the effects of energy transfer within the aggregate bridge between the donor and acceptor are evaluated.« less

Authors:
 [1];  [2];  [3];  [2];  [3]
  1. Arizona State Univ., Tempe, AZ (United States). Center for Innovations in Medicine at the Biodesign Inst.; National Inst. of Technology Tiruchirappalli,Tamil Nadu (Indian)
  2. Arizona State Univ., Tempe, AZ (United States). Center for Molecular Design and Biomimetics at the Biodesign Inst., and School of Molecular Sciences
  3. Arizona State Univ., Tempe, AZ (United States). Center for Innovations in Medicine at the Biodesign Inst., and School of Molecular Sciences
Publication Date:
Research Org.:
Arizona State Univ., Tempe, AZ (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1507096
Grant/Contract Number:  
SC0016353
Resource Type:
Accepted Manuscript
Journal Name:
Bioconjugate Chemistry
Additional Journal Information:
Journal Name: Bioconjugate Chemistry; Journal ID: ISSN 1043-1802
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mandal, Sarthak, Zhou, Xu, Lin, Su, Yan, Hao, and Woodbury, Neal W. Directed Energy Transfer through DNA-templated J-aggregates. United States: N. p., 2019. Web. doi:10.1021/acs.bioconjchem.9b00043.
Mandal, Sarthak, Zhou, Xu, Lin, Su, Yan, Hao, & Woodbury, Neal W. Directed Energy Transfer through DNA-templated J-aggregates. United States. doi:10.1021/acs.bioconjchem.9b00043.
Mandal, Sarthak, Zhou, Xu, Lin, Su, Yan, Hao, and Woodbury, Neal W. Mon . "Directed Energy Transfer through DNA-templated J-aggregates". United States. doi:10.1021/acs.bioconjchem.9b00043.
@article{osti_1507096,
title = {Directed Energy Transfer through DNA-templated J-aggregates},
author = {Mandal, Sarthak and Zhou, Xu and Lin, Su and Yan, Hao and Woodbury, Neal W.},
abstractNote = {Strongly coupled molecular dye aggregates have unique optoelectronic properties that often resemble those of light harvesting complexes found in nature. The exciton dynamics in coupled dye aggregates could enhance the long-range transfer of optical excitation energy with high efficiency. In principle, dye aggregates could serve as important components in molecular-scale photonic devices, however, rational design of these coupled dye aggregates with precise control over their organization, interactions and dynamics remains a challenge. DNA nanotechnology has recently been used to build an excitonic circuit by organizing pseudoisocyanine (PIC) dyes forming J-aggregates on the templates of poly(dA)-poly(dT) DNA duplexes. Here, the excitonic properties of the PIC J-aggregates on DNA are characterized spectroscopically in detail using poly(dA)-poly(dT) tract lengths of 24 and 48 base pairs. The excitonic properties of these DNA templated dye assemblies depend on the length and sequence of the DNA template. The incorporation of a gap of two GC base pairs between two segments of poly(dA)-poly(dT) DNA markedly reduces the delocalization of excitation in the J-aggregates.Using a quantum dot (QD) as the light absorber and energy donor and using Alexa Fluor 647 (AF647) as the energy acceptor, with a DNA-templated J-aggregate in between, significant energy transfer from QD to AF647 is observed over a distance far longer than possible without the aggregate bridge. By comparing the efficiency of energy transfer through a continuous J-aggregate with the efficiency when the aggregate has a discontinuity in the middle, the effects of energy transfer within the aggregate bridge between the donor and acceptor are evaluated.},
doi = {10.1021/acs.bioconjchem.9b00043},
journal = {Bioconjugate Chemistry},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on April 15, 2020
Publisher's Version of Record

Save / Share: