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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 upconversion via upconversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based upconversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an upconversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy upconversion 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 upconversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.
Highlights
IntroductionExcitons are funneled down an energy gradient created by an array of fluorophores possessing successively lower excitation energies
In many nanophotonic systems, excitons are funneled down an energy gradient created by an array of fluorophores possessing successively lower excitation energies
The state of the Förster resonant energy transfer (FRET) system was monitored in two ways after each switching event via fluorescence spectroscopy under conditions of continuous 980 nm excitation
Summary
Excitons are funneled down an energy gradient created by an array of fluorophores possessing successively lower excitation energies. Examples of such excitonic systems include light harvesting antennae in higher plants [1, 2], certain bacteria [3, 4], synthetic waveguides [5, 6], switches, and logic gates [7,8,9]. The efficiencies of upconversion nanoparticles (UCNPs) continue to improve [17], which offers an opportunity to pursue energy upconversion in artificial excitonic systems including excitonic wires, switches, and light harvesting antennae. Further development of UCNP systems may provide significant advancements in these nanomedicine and optoelectronics applications
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