Zhao Caibin, Ge Hongguang, Jin Lingxia, Zhang Qiang, Wang Zhanling, Wang Wenliang, Yin Shiwei
Shaanxi Province Key Laboratory of Catalytic Foundations and Applications, School of Chemical and Environmental Science, Shaanxi University of Technology, Hanzhong, 723000, China.
School of Mechanical Engineering, Shaanxi University of Technology, Hanzhong, 723000, China.
J Mol Model. 2016 Oct;22(10):241. doi: 10.1007/s00894-016-3117-7. Epub 2016 Sep 19.
Designing and synthesizing novel electron-donor polymers with the high photovoltaic performances has remained a major challenge and hot issue in organic electronics. In this work, the exciton-dissociation (k dis ) and charge-recombination (k rec ) rates for the PC61BM-PTDPPSe system as a promising polymer-based solar cell candidate have been theoretically investigated by means of density functional theory (DFT) calculations coupled with the non-adiabatic Marcus charge transfer model. Moreover, a series of regression analysis has been carried out to explore the rational structure-property relationship. Results reveal that the PC61BM-PTDPPSe system possesses the large open-circuit voltage (0.77 V), middle-sized exiton binding energy (0.457 eV), and relatively small reorganization energies in exciton-dissociation (0.273 eV) and charge-recombination (0.530 eV) processes. With the Marcus model, the k dis , k rec , and the radiative decay rate (k s ), are estimated to be 3.167×10(11) s(-1), 3.767×10(10) s(-1), and 7.930×10(8) s(-1) respectively in the PC61BM-PTDPPSe interface. Comparably, the k dis is as 1∼3 orders of magnitude larger than the k rec and the k s , which indicates a fast and efficient photoinduced exciton-dissociation process in the PC61BM-PTDPPSe interface. Graphical Abstract PTDPPSe is predicted to be a promising electron donor polymer, and the PC61BM-PTDPPSe system is worthy of further device research by experiments.
设计并合成具有高光伏性能的新型电子给体聚合物一直是有机电子学领域的一项重大挑战和热点问题。在本工作中，通过密度泛函理论（DFT）计算结合非绝热马库斯电荷转移模型，对作为一种有前景的聚合物基太阳能电池候选体系的PC61BM - PTDPPSe体系的激子解离（k dis）和电荷复合（k rec）速率进行了理论研究。此外，还进行了一系列回归分析以探索合理的结构 - 性能关系。结果表明，PC61BM - PTDPPSe体系具有较大的开路电压（0.77 V）、中等大小的激子结合能（0.457 eV），以及在激子解离（0.273 eV）和电荷复合（0.530 eV）过程中相对较小的重组能。利用马库斯模型，在PC61BM - PTDPPSe界面处，k dis、k rec和辐射衰减速率（k s）分别估计为3.167×10(11) s(-1)、3.767×10(10) s(-1)和7.930×10(8) s(-1)。相比之下，k dis比k rec和k s大1至3个数量级，这表明在PC61BM - PTDPPSe界面处存在快速且高效的光致激子解离过程。图形摘要PTDPPSe被预测为一种有前景的电子给体聚合物，PC61BM - PTDPPSe体系值得通过实验进行进一步的器件研究。
