Accelerating FRET between Near-Infrared Emitting Quantum Dots Using a Molecular J-Aggregate as an Exciton Bridge

Chen Wang, Emily A. Weiss

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

Fast energy transfer (EnT) among quantum dots (QDs) with near-infrared (NIR) emission is essential for fully exploiting their light harvesting and photon downconversion (multiexciton generation) abilities. This paper demonstrates a relayed EnT mechanism that accelerates the migration of NIR excitons between PbS QDs by a factor of 20 from that of one-step EnT through a polyelectrolyte and even a factor of ∼2 from that of one-step EnT between QDs in direct contact, by employing a J-aggregate (J-agg) of a cyanine dye as an exciton bridge. The donor QDs, acceptor QDs, and J-agg are electrostatically assembled into a sandwich structure with layer-by-layer deposition. Estimates of EnT rate and yield from transient and steady-state absorption and photoluminescence spectroscopies show that the rate-limiting step in the relay is EnT from the donor QD to the J-agg, while EnT from the J-agg to the acceptor QD occurs in <10 ps. A comparison of this system to the analogous solution-phase system suggests that the overall donor-to-acceptor EnT yield in the relay (18%) can be improved by depositing the J-agg with more intermolecular order. This work demonstrates the viability of relayed EnT through a molecular bridge as a strategy for accelerating long-distance exciton migration in assemblies of QDs, in particular in the near-infrared.

Original languageEnglish
Pages (from-to)5666-5671
Number of pages6
JournalNano letters
Volume17
Issue number9
DOIs
Publication statusPublished - Sep 13 2017

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Keywords

  • FRET
  • J-aggregate
  • PbS quantum dots
  • cyanine dye
  • layer-by-layer
  • near-infrared

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

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