期刊
NANO LETTERS
卷 14, 期 3, 页码 1263-1269出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl4041687
关键词
Quantum dots; transient absorption spectroscopy; electron transfer; Auger; Marcus theory
类别
资金
- Office of Basic Energy Sciences of the U.S. Department of Energy [DE-FG02-12ER16347, DE-SC0006527]
- KAKENHI [24750016]
- Royal Society under the URF scheme
- Grants-in-Aid for Scientific Research [24750016] Funding Source: KAKEN
Although quantum confined nanomaterials, such as quantum dots (QDs) have emerged as a new class of light harvesting and charge separation materials for solar energy conversion, theoretical models for describing photoinduced charge transfer from these materials remain unclear. In this paper, we show that the rate of photoinduced electron transfer from QDs (CdS, CdSe, and CdTe) to molecular acceptors (anthraquinone, methylviologen, and methylene blue) increases at decreasing QD size (and increasing driving force), showing a lack of Marcus inverted regime behavior over an apparent driving force range of similar to 0-1.3 V. We account for this unusual driving force dependence by proposing an Auger-assisted electron transfer model in which the transfer of the electron can be coupled to the excitation of the hole, circumventing the unfavorable Franck-Condon overlap in the Marcus inverted regime. This model is supported by computational studies of electron transfer and trapping processes in model QD-acceptor complexes.
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