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Mechanistic Understanding and Rational Design of Quantum Dot/Mediator Interfaces for Efficient Photon Upconversion.

Zihao Xu1, Zhiyuan Huang2, Tao Jin1

  • 1Department of Chemistry, Emory University, Atlanta, Georgia 30322, United States.

Accounts of Chemical Research
|November 3, 2020
PubMed
Summary

Semiconductor-nanocrystal-sensitized upconversion systems utilize photosensitizers, mediators, and emitters to convert low-energy photons to higher-energy ones. Optimizing triplet energy transfer between these components is key to enhancing quantum efficiency in these advanced photon upconversion technologies.

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Area of Science:

  • Materials Science
  • Nanotechnology
  • Photochemistry

Background:

  • Three-component upconversion systems, comprising a photosensitizer, mediator, and emitter, are crucial for photon energy conversion.
  • Semiconductor nanocrystals, particularly quantum dots (QDs), offer tunable band gaps and high triplet exciton yields, making them effective photosensitizers.
  • Efficient triplet energy transfer (TET) between components is essential for maximizing quantum efficiency (QE) and anti-Stokes shift.

Purpose of the Study:

  • To review chalcogenide QD-based photon upconversion systems, focusing on the mechanistic aspects of triplet energy transfer.
  • To identify rate-limiting factors and loss pathways in QD-sensitized upconversion systems using time-resolved spectroscopy.
  • To provide a framework for optimizing sensitizer, mediator, and emitter components for improved upconversion performance.

Main Methods:

  • Utilized time-resolved spectroscopy to investigate the kinetics and efficiency of triplet energy transfer steps.
  • Focused on near-infrared (NIR) to visible (VIS) PbS-tetracene systems for systematic control over QD, mediator, and emitter properties.
  • Analyzed Dexter-type triplet energy transfer (TET) and charge transfer (CT) pathways.

Main Results:

  • Mediator triplet state formation is primarily via direct TET from the QD, influenced by mediator molecule density.
  • Charge transfer (CT) is an identified loss pathway that can be minimized by QD surface passivation.
  • The second TET rate is limited by the mediator's triplet lifetime, not diffusion, highlighting it as a key bottleneck.

Conclusions:

  • Optimized energy cascades and minimized energy losses are critical for efficient QD-sensitized photon upconversion.
  • Understanding and controlling the two sequential triplet energy transfer steps are essential for improving overall quantum efficiency.
  • The findings are generalizable to other QD-sensitized systems and related phenomena like singlet fission.