Photoinduced Electron Transfer in CdSe/ZnS Quantum Dot鈥揊ullerene Hybrids

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• 作者：Kirsi Virkki ; Sinem Demir ; Helge Lemmetyinen ; Nikolai V. Tkachenko
• 刊名：Journal of Physical Chemistry C
• 出版年：2015
• 出版时间：August 6, 2015
• 年：2015
• 卷：119
• 期：31
• 页码：17561-17572
• 全文大小：608K
• ISSN：1932-7455

文摘

Photoinduced electron transfer (ET) in CdSe/ZnS core鈥搒hell quantum dot (QD) 鈥?fullerene (COOH鈥揅₆₀) hybrids was studied by the means of time-resolved emission and absorption spectroscopy techniques. A series of four QDs with emission in the range 540鈥?30 nm was employed to investigate the dependence of the electron transfer rate on the QD size. Emission of the QDs is quenched upon hybrid formation, and the quenching mechanism is identified as photoinduced electron transfer from the QD to the fullerene moiety due to the fullerene anion signature observed in transient absorption. In order to obtain quantitative information on the ET reaction, several kinetic data analysis techniques were used, including a conventional multiexponential fitting and a maximum entropy method for emission decay analysis, as well as a distributed decay model based on the Poisson distribution of fullerenes in the hybrids. The latter gradually simplifies the interpretation of the transient absorption spectra and indicates that the spectra of QD cations are essentially similar to those of neutral QDs, differing only by a minor decrease in the intensity and broadening. Furthermore, only a minor decrease in the ET rate with the increasing QD size was observed, the time constants being in the range 100鈥?00 ps for all studied QDs. The charge recombination is extended to 10 ns or longer for all hybrids.