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Related Concept Videos

Electron Carriers01:24

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Electron carriers can be thought of as electron shuttles. These compounds can easily accept electrons (i.e., be reduced) or lose them (i.e., be oxidized). They play an essential role in energy production because cellular respiration is contingent on the flow of electrons.
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Carrier generation is the process by which electron-hole pairs (EHPs) are created within the semiconductor. In direct-bandgap semiconductors, such as gallium arsenide (GaAs), this occurs efficiently when energy absorption prompts valence electrons to leap into the conduction band, leaving behind holes.
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Integrating a Triplet-triplet Annihilation Up-conversion System to Enhance Dye-sensitized Solar Cell Response to Sub-bandgap Light
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Sequential Carrier Transfer Can Accelerate Triplet Energy Transfer from Functionalized CdSe Nanocrystals.

Minhal Hasham1, Pournima Narayanan1, Francisco Yarur Villanueva1

  • 1Department of Chemistry, University of Toronto, Toronto, Ontario M5S 3H6, Canada.

The Journal of Physical Chemistry Letters
|February 13, 2023
PubMed
Summary

We studied how light energy is converted using cadmium selenide nanocrystals (CdSe NCs) and transmitter ligands. Lowering energy barriers significantly speeds up energy transfer, making sequential transfer the dominant process for efficient light conversion.

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Area of Science:

  • Materials Science
  • Photochemistry
  • Nanotechnology

Background:

  • Triplet-fusion upconversion converts long-wavelength light to higher-energy photons.
  • Nanocrystal (NC)-sensitized upconversion is an emerging strategy for this conversion.
  • Understanding energy transfer dynamics in functionalized NCs is crucial for optimizing performance.

Purpose of the Study:

  • To investigate the photophysics of energy transfer from tailor-functionalized cadmium selenide (CdSe) NCs to surface-anchored transmitter ligands.
  • To elucidate the mechanisms of energy transfer, distinguishing between correlated exciton transfer and sequential carrier hops.
  • To determine how NC size and energy barriers influence the kinetics and dominant pathways of energy transfer.

Main Methods:

  • Fabrication of tailor-functionalized CdSe NCs with varying sizes.
  • Spectroscopic analysis to probe energy transfer pathways (exciton transfer vs. carrier hops).
  • Transient photoluminescence spectroscopy to study quenching dynamics of band-edge and trap states.

Main Results:

  • Energy transfer rate (kquench) increased significantly (0.0096 to 0.064 ns-1 ligand-1) when the hole-first sequential transfer barrier decreased from 100 ± 25 meV to 50 ± 25 meV.
  • This acceleration was 5.1 times greater than expected from carrier wave function leakage alone, indicating a shift in dominant mechanism.
  • Both NC band-edge and trap states were efficiently quenched (up to ~98% for sequential transfer) with matched long-term dynamics (>300 ns).

Conclusions:

  • Sequential carrier transfer becomes kinetically dominant over correlated exciton transfer when the energy barrier is sufficiently lowered.
  • Functionalization effectively quenches both band-edge and trap states in CdSe NCs.
  • A dynamic quasi-equilibrium facilitates efficient photoexcitation extraction, even from initially trapped states, crucial for upconversion applications.