Title: Efficient Long-range, Directional Energy Transfer through DNA-Templated Dye Aggregates

Abstract

The benzothiazole cyanine dye, K21, forms dye aggregates on double stranded DNA (dsDNA) templates. These aggregates exhibit a red-shifted absorption band, enhanced fluorescence emission and an increased fluorescence lifetime, all indicating strong excitonic coupling among the dye molecules. K21 aggregate formation on dsDNA is only weakly sequence dependent, providing a flexible approach that is adaptable to many different DNA nanostructures. Donor (D) – bridge (B) – Acceptor (A) complexes consisting of Alexa Fluor 350 as the donor, a 30 bp (9.7 nm) DNA templated K21 aggregate as the bridge and Alexa Fluor 555 as the acceptor show an overall donor to acceptor energy transfer efficiency of ~60%, with the loss of excitation energy being almost exclusively at the donor-bridge junction (63%). There was almost no excitation energy loss due to transfer through the aggregate bridge and the transfer efficiency from the aggregate to the acceptor was about 96%. By comparing the energy transfer in templated aggregates at several lengths up to 32 nm, the loss of energy per nanometer through the K21 aggregate bridge was determined to be <1%, suggesting that it should be possible to construct structures that use much longer energy transfer “wires” for light-harvesting applications in photonicmore » systems.« less

Authors:

Zhou, Xu ^[1]; Mandal, Sarthak ^[2]; Jiang, Shuoxing ^[3]; Lin, Su ^[4]; Yang, Jianzhong ^[5]; Liu, Yan ^[1]; Whitten, David G. ^[5]; Woodbury, Neal W. ^[4]; Yan, Hao ^[1]

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+ Show Author Affiliations

1. Arizona State Univ., Tempe, AZ (United States). Center for Molecular Design and Biomimetics at the Biodesign Inst., and School of Molecular Sciences
2. Arizona State Univ., Tempe, AZ (United States). Center for Innovations in Medicine at the Biodesign Inst.; National Inst. of Technology Tiruchirappalli, Tamil Nadu (India). Dept. of Chemistry
3. Arizona State Univ., Tempe, AZ (United States). Center for Molecular Design and Biomimetics at the Biodesign Inst.
4. Arizona State Univ., Tempe, AZ (United States). Center for Innovations in Medicine at the Biodesign Inst.; Arizona State Univ., Tempe, AZ (United States). School of Molecular Sciences
5. Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering

Publication Date:

2019-04-16

Research Org.:

Arizona State Univ., Tempe, AZ (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1507100

Grant/Contract Number:  

SC0016353

Resource Type:

Accepted Manuscript

Journal Name:

Journal of the American Chemical Society

Additional Journal Information:

Journal Volume: 141; Journal Issue: 21; Journal ID: ISSN 0002-7863

Publisher:

American Chemical Society (ACS)

Country of Publication:

United States

Language:

English

Subject:

59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY