Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage

Justin Johnson, Jeffrey Blackburn, Gerard Carroll, Matthew Beard, John Anthony, Devin Granger, Dylan Arias, Daniel Kroupa

Research output: Contribution to journalArticlepeer-review

61 Scopus Citations

Abstract

We have prepared a series of samples with the ligand 6,13-bistri(iso-propyl)silylethynyl tetracene 2-carboxylic acid (TIPS-Tc-COOH) attached to PbS quantum dot (QD) samples of three different sizes in order to monitor and control the extent and time scales of energy flow after photoexcitation. Fast energy transfer (?1 ps) to the PbS QD occurs upon direct excitation of the ligand for all samples. The largest size QD maintains the microsecond exciton lifetime characteristic of the as-prepared oleate terminated PbS QDs. However, two smaller QD sizes with lowest exciton energies similar to or larger than the TIPS-Tc-COO? triplet energy undergo energy transfer between QD core and ligand triplet on nanosecond to microsecond timescales. For the intermediate size QDs in particular, energy can be recycled many times between ligand and core, but the triplet remains the dominant excited species at long times, living for ?3 μs for fully exchanged QDs and up to 30 μs for partial ligand exchange, which is revealed as a method for controlling the triplet lifetime. A unique upconverted luminescence spectrum is observed that results from annihilation of triplets after exclusive excitation of the QD core.

Original languageAmerican English
Pages (from-to)865-873
Number of pages9
JournalNano Letters
Volume18
Issue number2
DOIs
StatePublished - 2018

Bibliographical note

Publisher Copyright:
© 2018 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-70058

Keywords

  • energy transfer
  • photoluminescence
  • quantum dots
  • solar-photochemistry
  • triplet
  • upconversion

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