期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 19, 页码 6163-6170出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b13386
关键词
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资金
- U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001059]
- Camille and Henry Dreyfus Postdoctoral Program in Environmental Chemistry
- Graduate Research Fellowship (GRF) from the National Science Foundation
- Ryan Fellowship
- NU International Institute for Nanotechnology
- Fulbright Scholars Program
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)) (ExBox(4+)) to form both the ExBox(3+center dot) and the doubly reduced ExBox(2(+center dot))) 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 similar to 5 ps, which leads to a mixture of redox states of the acceptor ligand. The doubly reduced ExBox(2(+center dot)) state has a lifetime of similar to 10 ns, while CdS+center dot:ExBox(3+center dot) recombines with multiple time constants, the longest of which is similar to 300 ps. The long-lived charge separation and ability to accumulate multiple charges on ExBox(4+) demonstrate the potential of the CdS:ExBox(4+) complex to serve as a platform for two-electron photocatalysis.
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