DNA-mediated excitonic upconversion FRET switching

Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.

doi:10.1088/1367-2630/17/11/115007

Title: DNA-mediated excitonic upconversion FRET switching

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Abstract

Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy up conversion via up conversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based up conversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an up conversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy up conversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy up conversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.

Authors:

Kellis, Donald L. ^[1]; Rehn, Sarah M. ^[2]; Cannon, Brittany L. ^[1]; Davis, Paul H. ^[1]; Graugnard, Elton ^[1]; Lee, Jeunghoon ^[3]; Yurke, Bernard ^[4]; Knowlton, William B. ^[4]

Boise State Univ., ID (United States). Department of Materials Science and Engineering
Boise State Univ., ID (United States). Department of Chemistry and Biochemistry
Boise State Univ., ID (United States). Department of Materials Science and Engineering; Boise State Univ., ID (United States). Department of Chemistry and Biochemistry
Boise State Univ., ID (United States). Department of Materials Science and Engineering; Boise State Univ., ID (United States). Department of Electrical and Computer Engineering

Publication Date:: Tue Nov 17 00:00:00 EST 2015

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

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

OSTI Identifier:: 1241131

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: New Journal of Physics

Additional Journal Information:: Journal Volume: 17; Journal Issue: 11; Journal ID: ISSN 1367-2630

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; upconverting nanoparticles; FRET,DNAnanotechnology; excitonics; strand displacement; excitonic switch

Citation Formats


                    Kellis, Donald L., Rehn, Sarah M., Cannon, Brittany L., Davis, Paul H., Graugnard, Elton, Lee, Jeunghoon, Yurke, Bernard, and Knowlton, William B. DNA-mediated excitonic upconversion FRET switching.  United States: N. p., 2015. 
Web.  doi:10.1088/1367-2630/17/11/115007.

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                    Kellis, Donald L., Rehn, Sarah M., Cannon, Brittany L., Davis, Paul H., Graugnard, Elton, Lee, Jeunghoon, Yurke, Bernard, & Knowlton, William B. DNA-mediated excitonic upconversion FRET switching.  United States.  https://doi.org/10.1088/1367-2630/17/11/115007

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                    Kellis, Donald L., Rehn, Sarah M., Cannon, Brittany L., Davis, Paul H., Graugnard, Elton, Lee, Jeunghoon, Yurke, Bernard, and Knowlton, William B. Tue .  
"DNA-mediated excitonic upconversion FRET switching".  United States.  https://doi.org/10.1088/1367-2630/17/11/115007.  https://www.osti.gov/servlets/purl/1241131.

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@article{osti_1241131,

  title        = {DNA-mediated excitonic upconversion FRET switching},

  author       = {Kellis, Donald L. and Rehn, Sarah M. and Cannon, Brittany L. and Davis, Paul H. and Graugnard, Elton and Lee, Jeunghoon and Yurke, Bernard and Knowlton, William B.},

  abstractNote = {Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy up conversion via up conversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based up conversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an up conversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy up conversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy up conversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.},

  doi          = {10.1088/1367-2630/17/11/115007},

  journal      = {New Journal of Physics},

  number       = 11,

  volume       = 17,

  place        = {United States},

  year         = {Tue Nov 17 00:00:00 EST 2015},

  month        = {Tue Nov 17 00:00:00 EST 2015}

}

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