Sub-Nanosecond Resonance Energy Transfer in the Near-Infrared within Self-Assembled Conjugates of PbS Quantum Dots and Cyanine Dye J-Aggregates

Chen Wang, Emily A Weiss

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

Energy transfer (EnT) of near-infrared (NIR) excitons enables applications in harvesting of solar energy and biological imaging. Fast exciton extraction from NIR-absorbing Pb-chalcogenide quantum dots (QDs) may allow utilization of the photon downconversion (multiple exciton generation) process that occurs in those QDs to amplify signal in QD-based sensors or photocurrent in QD-based photovoltaics. This paper describes subnanosecond extraction of NIR excitons from PbS QDs by adsorbed J-aggregates of cyanine dye in aqueous dispersions. The QD/J-aggregate complexes form through electrostatic self-assembly, and the rate and yield of EnT within the complexes can be optimized by adjusting spectral overlap between QD emission and the J-aggregate absorption, which are controlled by density of charged ligands on the QD surface and the pH. The primary EnT pathways have rate constants ranging from (800 ps)-1 to (2.2 ns)-1, which are 1-2 orders of magnitude faster than previously reported examples with PbS QDs as exciton donors. The fastest EnT process occurs in 90 ps and is potentially competitive with Auger recombination of biexcitonic states in PbS QDs.

Original languageEnglish
Pages (from-to)9557-9564
Number of pages8
JournalJournal of the American Chemical Society
Volume138
Issue number30
DOIs
Publication statusPublished - Aug 3 2016

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Quantum Dots
Energy Transfer
Energy transfer
Semiconductor quantum dots
Coloring Agents
Dyes
Infrared radiation
Excitons
Solar Energy
Static Electricity
Photocurrents
Dispersions
Photons
Self assembly
Solar energy
Genetic Recombination
Electrostatics
Rate constants
Ligands
LDS 751

ASJC Scopus subject areas

  • Catalysis
  • Biochemistry
  • Chemistry(all)
  • Colloid and Surface Chemistry

Cite this

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title = "Sub-Nanosecond Resonance Energy Transfer in the Near-Infrared within Self-Assembled Conjugates of PbS Quantum Dots and Cyanine Dye J-Aggregates",
abstract = "Energy transfer (EnT) of near-infrared (NIR) excitons enables applications in harvesting of solar energy and biological imaging. Fast exciton extraction from NIR-absorbing Pb-chalcogenide quantum dots (QDs) may allow utilization of the photon downconversion (multiple exciton generation) process that occurs in those QDs to amplify signal in QD-based sensors or photocurrent in QD-based photovoltaics. This paper describes subnanosecond extraction of NIR excitons from PbS QDs by adsorbed J-aggregates of cyanine dye in aqueous dispersions. The QD/J-aggregate complexes form through electrostatic self-assembly, and the rate and yield of EnT within the complexes can be optimized by adjusting spectral overlap between QD emission and the J-aggregate absorption, which are controlled by density of charged ligands on the QD surface and the pH. The primary EnT pathways have rate constants ranging from (800 ps)-1 to (2.2 ns)-1, which are 1-2 orders of magnitude faster than previously reported examples with PbS QDs as exciton donors. The fastest EnT process occurs in 90 ps and is potentially competitive with Auger recombination of biexcitonic states in PbS QDs.",
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N2 - Energy transfer (EnT) of near-infrared (NIR) excitons enables applications in harvesting of solar energy and biological imaging. Fast exciton extraction from NIR-absorbing Pb-chalcogenide quantum dots (QDs) may allow utilization of the photon downconversion (multiple exciton generation) process that occurs in those QDs to amplify signal in QD-based sensors or photocurrent in QD-based photovoltaics. This paper describes subnanosecond extraction of NIR excitons from PbS QDs by adsorbed J-aggregates of cyanine dye in aqueous dispersions. The QD/J-aggregate complexes form through electrostatic self-assembly, and the rate and yield of EnT within the complexes can be optimized by adjusting spectral overlap between QD emission and the J-aggregate absorption, which are controlled by density of charged ligands on the QD surface and the pH. The primary EnT pathways have rate constants ranging from (800 ps)-1 to (2.2 ns)-1, which are 1-2 orders of magnitude faster than previously reported examples with PbS QDs as exciton donors. The fastest EnT process occurs in 90 ps and is potentially competitive with Auger recombination of biexcitonic states in PbS QDs.

AB - Energy transfer (EnT) of near-infrared (NIR) excitons enables applications in harvesting of solar energy and biological imaging. Fast exciton extraction from NIR-absorbing Pb-chalcogenide quantum dots (QDs) may allow utilization of the photon downconversion (multiple exciton generation) process that occurs in those QDs to amplify signal in QD-based sensors or photocurrent in QD-based photovoltaics. This paper describes subnanosecond extraction of NIR excitons from PbS QDs by adsorbed J-aggregates of cyanine dye in aqueous dispersions. The QD/J-aggregate complexes form through electrostatic self-assembly, and the rate and yield of EnT within the complexes can be optimized by adjusting spectral overlap between QD emission and the J-aggregate absorption, which are controlled by density of charged ligands on the QD surface and the pH. The primary EnT pathways have rate constants ranging from (800 ps)-1 to (2.2 ns)-1, which are 1-2 orders of magnitude faster than previously reported examples with PbS QDs as exciton donors. The fastest EnT process occurs in 90 ps and is potentially competitive with Auger recombination of biexcitonic states in PbS QDs.

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