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

doi:10.1021/jacs.5b13386

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

Northwestern University

Research output: Contribution to journal › Article › peer-review

31 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 ExBox^3+• and the doubly reduced ExBox^2(+•) 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 ExBox^2(+•) state has a lifetime of ∼10 ns, while CdS^+•:ExBox^3+• 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 language	English
Pages (from-to)	6163-6170
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	138
Issue number	19
DOIs	https://doi.org/10.1021/jacs.5b13386
Publication status	Published - May 18 2016

ASJC Scopus subject areas

Chemistry(all)
Catalysis
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.5b13386

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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 journal › Article › peer-review

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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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.",

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