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 language | English |
|---|---|
| Pages (from-to) | 6163-6170 |
| Number of pages | 8 |
| Journal | Journal of the American Chemical Society |
| Volume | 138 |
| Issue number | 19 |
| DOIs | |
| Publication status | Published - May 18 2016 |
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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 journal › Article
}
TY - JOUR
T1 - Ultrafast Two-Electron Transfer in a CdS Quantum Dot-Extended-Viologen Cyclophane Complex
AU - Young, Ryan M.
AU - Jensen, Stephen C.
AU - Edme, Kedy
AU - Wu, Yilei
AU - Krzyaniak, Matthew D.
AU - Vermeulen, Nicolaas A.
AU - Dale, Edward J.
AU - Stoddart, J. Fraser
AU - Weiss, Emily A
AU - Wasielewski, Michael R
AU - Co, Dick T
PY - 2016/5/18
Y1 - 2016/5/18
N2 - 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.
AB - 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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UR - http://www.scopus.com/inward/citedby.url?scp=84971220423&partnerID=8YFLogxK
U2 - 10.1021/jacs.5b13386
DO - 10.1021/jacs.5b13386
M3 - Article
AN - SCOPUS:84971220423
VL - 138
SP - 6163
EP - 6170
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 19
ER -