Ultrafast Dynamics of CdSe/ZnS Quantum Dots and Quantum
Dot-Acceptor Molecular Complexes
BAI Xi-lin1, 2, PENG Yue1, 2, ZHANG Xue-dong1, 2, GE Jing1, 2*
1. School of Physics and Information Engineering, Shanxi Normal University, Taiyuan 030031, China
2. Key Laboratory of Spectral Measurement and Analysis of Shanxi Province, Taiyuan 030031, China
Abstract:QDs are a new class of semiconductor light-emitting nanomaterials, which have attracted much attention due to their unique optical properties such as adjustable luminous colorand size, wide excitation spectrum, narrow emission spectrum, etc. It is the ideal material for photovoltaic device applications in which nuclear/shell QD has better optical performance than single QD. For instance, type I nuclear/shell QD solar cell devices show higher stability and conversion efficiency in quantum dot-sensitized solar cells. Nevertheless, how the interfacial process and recombination kinetics affect the performance of devices have been the focus of attention, and the lack of related cognition has hindered the further development of quantum dot photovoltaic devices. A comprehensive study on carrier dynamics of the topical CdSe/ZnS QDs and QD-acceptor (1-chloroanthraquinone (1-CAQ), anthraquinone (AQ), and methyl viologen (MV2+)) complexes are performed employing the femtosecond time-resolved transient absorption (TA) spectroscopy and quantum chemical calculations. As indicated by the spectroscopic analysis, the fastest ET and AR processes occurred in QD-MV2+ complexes, and the ET rate was positively correlated with the AR rate. In addition, the bandgap of electron acceptor molecules and the driving force were demonstrated as crucial factors affecting the rate of the ET process according to Marcus's ET theory combined with density function calculation.This study will provide new insights into the selection of electron acceptor molecules, which will be essential in improving the design of photovoltaic devices.
Key words:Quantum dots; Transient absorption spectroscopy; Density functional theory; Electron transfer
[1] Ocak I, Kara H E S. Journal of Luminescence, 2018, 197(5): 112.
[2] Baruah Sunandan, Sinha Sudarson Sekhar, Ghosh Barnali, et al. Journal of Applied Physics, 2009, 105(7): 074308.
[3] Shulga Artem G, Kahmann Simon, Dirin Dmitry N, et al. ACS Nano, 2018, 12(12): 12805.
[4] Wu Kaifeng, Lian Tianquan. Chemical Society Reviews, 2016, 45(14): 3781.
[5] Li Yuanzuo, Xu Beibei, Song Peng, et al. The Journal of Physical Chemistry C, 2017, 121(23): 12546.
[6] Zhu Haiming, Song Nianhui, Lian Tianquan. Journal of the American Chemical Society, 2010, 132(42): 15038.
[7] Kaledin Alexey L, Lian Tianquan, Hill Craig L, et al. The Journal of Physical Chemistry B, 2015, 119(24): 7651.
[8] Zhao Huifang, Li You, Diao Lihe, et al. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 2019, 218(13): 237.
[9] Scholz Frank, Dworak Lars, Matylitsky Victor V, et al. ChemPhysChem, 2011, 12(12): 2255.
[10] Cui Shicong, Tachikawa Takashi, Fujitsuka Mamoru, et al. The Journal of Physical Chemistry C, 2010, 114(2): 1217.
[11] Park Young-Shin, Bae Wan Ki, Padilha Lazaro A, et al. Nano Letters, 2014, 14(2): 396.
[12] Ge Jing, Zhang Qun, Jiang Jun, et al. Physical Chemistry Chemical Physics, 2015, 17(19): 13129.
[13] QIN Chao-chao, LIU Hua, ZHOU Zhong-po(秦朝朝,刘 华,周忠坡). Spectroscopy and Spectral Analysis(光谱学与光谱分析), 2021, 41(6): 1695.
[14] WAN Hao-yu, ZHOU Zi-xiong, WU Jun-biao, et al(万浩宇,周子雄,吴俊彪,等). Spectroscopy and Spectral Analysis(光谱学与光谱分析), 2022, 42(2): 368.
[15] Zhou Panwang, Liu Jianyong, Yang Songqiu, et al. Physical Chemistry Chemical Physics, 2012, 14(43): 15191.
[16] Huang Jier, Huang Zhuangqun, Yang Ye, et al. Journal of the American Chemical Society, 2010, 132(13): 4858.
[17] Gao Yunan, Sandeep C S Suchand, Schins Juleon M, et al. Nature Communications, 2013, 4: 2329.
[18] Masteri-Farahani M, Khademabbasi K. Journal of Luminescence, 2018, 204(12): 130.
[19] Zhao Huifang, Sun Chaofan, Yin Hang, et al. Scientific Reports, 2019, 9: 7756.
[20] Shi Xiaolong, Yang Yanhui, Wang Lihai, et al. The Journal of Physical Chemistry C, 2019, 123(7): 4007.