Reevaluating the effects of reorganization energy on electron transfer rate for quantum dot-molecular acceptor complexes in different solvents.

Authors:
Huifang Zhao
Huifang Zhao
the Affiliated Cancer Hospital of Zhengzhou University
You Li
You Li
Center for Studies of Psychological Application and School of Psychology
Fort Lauderdale | United States
Chaofan Sun
Chaofan Sun
School of Stomatology
Ying Shi
Ying Shi
Zhejiang University
China

Spectrochim Acta A Mol Biomol Spectrosc 2019 Jul 11;218:237-242. Epub 2019 Apr 11.

Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012, China. Electronic address:

The electron transfer (ET) rate in quantum dot (QD)-molecular acceptor systems is dependent upon system reorganization energy (RE, λ), which comprises contributions from solvent (λ) and reactants (λ). However, to date, the effect of λ on ET rate has been largely ignored. Herein, the ET from CdSe/ZnS QDs to 1-chloroanthraquinone (1-CAQ) in different solvents was investigated using ultrafast transient absorption spectroscopy as a means to evaluate the effect of λ on ET rate. The results revealed that ET rate is strongly solvent dependent. Amazingly, the ET rate in carbon disulfide is 300-times higher than that in n-dodecane. Theoretical calculations indicated that the λ contribution from 1-CAQ alone accounts for a large proportion of system RE and varies greatly in different solvents. Furthermore, the ET rate increases first and, then, decreases with the λ value in different solvents. This trend was interpreted consistently in terms of Marcus theory by adding λ to λ for different solvents. Thus, our present work demonstrates that the RE of the acceptor molecule has a non-negligible effect on ET rate, providing new insight into the mechanisms of ET process and for the development of QD-based devices.

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Source
http://dx.doi.org/10.1016/j.saa.2019.04.016DOI Listing
July 2019

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