Directed Energy Transfer through DNA-templated J-aggregates

Mandal, Sarthak; Zhou, Xu; Lin, Su; Yan, Hao; Woodbury, Neal W.

doi:10.1021/acs.bioconjchem.9b00043

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

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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 »« less

Authors:

Mandal, Sarthak ^[1]; Zhou, Xu ^[2]; Lin, Su ^[3]; Yan, Hao ^[2]; Woodbury, Neal W. ^[3]

Arizona State Univ., Tempe, AZ (United States). Center for Innovations in Medicine at the Biodesign Inst.; National Inst. of Technology Tiruchirappalli,Tamil Nadu (Indian)
Arizona State Univ., Tempe, AZ (United States). Center for Molecular Design and Biomimetics at the Biodesign Inst., and School of Molecular Sciences
Arizona State Univ., Tempe, AZ (United States). Center for Innovations in Medicine at the Biodesign Inst., and School of Molecular Sciences

Publication Date:: Mon Apr 15 00:00:00 EDT 2019

Research Org.:: Arizona State Univ., Tempe, AZ (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1507096

Grant/Contract Number:: SC0016353

Resource Type:: Accepted Manuscript

Journal Name:: Bioconjugate Chemistry

Additional Journal Information:: Journal Volume: 30; Journal Issue: 7; 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.

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                    Mandal, Sarthak, Zhou, Xu, Lin, Su, Yan, Hao, & Woodbury, Neal W. Directed Energy Transfer through DNA-templated J-aggregates.  United States.  https://doi.org/10.1021/acs.bioconjchem.9b00043

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                    Mandal, Sarthak, Zhou, Xu, Lin, Su, Yan, Hao, and Woodbury, Neal W. Mon .  
"Directed Energy Transfer through DNA-templated J-aggregates".  United States.  https://doi.org/10.1021/acs.bioconjchem.9b00043.  https://www.osti.gov/servlets/purl/1507096.

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@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       = 7,

  volume       = 30,

  place        = {United States},

  year         = {Mon Apr 15 00:00:00 EDT 2019},

  month        = {Mon Apr 15 00:00:00 EDT 2019}

}

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