Ultrafast Two-Electron Transfer in a CdS Quantum Dot-Extended-Viologen Cyclophane Complex

Ryan M. Young, Stephen C. Jensen, Kedy Edme, Yilei Wu, Matthew D. Krzyaniak, Nicolaas A. Vermeulen, Edward J. Dale, J. Fraser Stoddart, Emily A Weiss, Michael R Wasielewski, Dick T Co

Research output: Contribution to journalArticle

20 Citations (Scopus)

Abstract

Time-resolved optical spectroscopies reveal multielectron transfer from the biexcitonic state of a CdS quantum dot to an adsorbed tetracationic compound cyclobis(4,4′-(1,4-phenylene) bipyridin-1-ium-1,4-phenylene-bis(methylene)) (ExBox4+) to form both the ExBox3+• and the doubly reduced ExBox2(+•) states from a single laser pulse. Electron transfer in the single-exciton regime occurs in 1 ps. At higher excitation powers the second electron transfer takes ∼5 ps, which leads to a mixture of redox states of the acceptor ligand. The doubly reduced ExBox2(+•) state has a lifetime of ∼10 ns, while CdS+•:ExBox3+• recombines with multiple time constants, the longest of which is ∼300 μs. The long-lived charge separation and ability to accumulate multiple charges on ExBox4+ demonstrate the potential of the CdS:ExBox4+ complex to serve as a platform for two-electron photocatalysis.

Original languageEnglish
Pages (from-to)6163-6170
Number of pages8
JournalJournal of the American Chemical Society
Volume138
Issue number19
DOIs
Publication statusPublished - May 18 2016

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Viologens
Quantum Dots
Semiconductor quantum dots
Electrons
Photocatalysis
Excitons
Oxidation-Reduction
Laser pulses
Spectrum Analysis
Lasers
Ligands

ASJC Scopus subject areas

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

Cite this

Ultrafast Two-Electron Transfer in a CdS Quantum Dot-Extended-Viologen Cyclophane Complex. / Young, Ryan M.; Jensen, Stephen C.; Edme, Kedy; Wu, Yilei; Krzyaniak, Matthew D.; Vermeulen, Nicolaas A.; Dale, Edward J.; Stoddart, J. Fraser; Weiss, Emily A; Wasielewski, Michael R; Co, Dick T.

In: Journal of the American Chemical Society, Vol. 138, No. 19, 18.05.2016, p. 6163-6170.

Research output: Contribution to journalArticle

Young, RM, Jensen, SC, Edme, K, Wu, Y, Krzyaniak, MD, Vermeulen, NA, Dale, EJ, Stoddart, JF, Weiss, EA, Wasielewski, MR & Co, DT 2016, 'Ultrafast Two-Electron Transfer in a CdS Quantum Dot-Extended-Viologen Cyclophane Complex', Journal of the American Chemical Society, vol. 138, no. 19, pp. 6163-6170. https://doi.org/10.1021/jacs.5b13386
Young, Ryan M. ; Jensen, Stephen C. ; Edme, Kedy ; Wu, Yilei ; Krzyaniak, Matthew D. ; Vermeulen, Nicolaas A. ; Dale, Edward J. ; Stoddart, J. Fraser ; Weiss, Emily A ; Wasielewski, Michael R ; Co, Dick T. / Ultrafast Two-Electron Transfer in a CdS Quantum Dot-Extended-Viologen Cyclophane Complex. In: Journal of the American Chemical Society. 2016 ; Vol. 138, No. 19. pp. 6163-6170.
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