State Key Laboratory of Physical Chemistry of Solid Surfaces and Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 360015, China.
Phys Chem Chem Phys. 2013 Sep 7;15(33):13844-51. doi: 10.1039/c3cp51019k. Epub 2013 May 22.
Plausible mechanisms of the ultrafast electron injection and the significant dependence of the power conversion efficiency on the anchor group for the triphenylamine-based dye-sensitized TiO2 solar cells have been explored by the density functional calculations. Calculations show that the ultrafast charge recombination on the surface trap state of the dye-sensitized TiO2 system can be ascribed to the lack of electron density on the carboxyl group of the A3 dye with the rhodanine group anchor. Predicted electronic and optical properties of the A1-3-adsorbed TiO2 system reveal that the direct electron injection arises from the electronic excitation from HOMO-1 of the dye to the conduction band bottom of TiO2. On the basis of the calculations, the electron density distributions of related frontier orbitals and energy bands of dyes and their adsorbed systems have been discussed, which play an important role in electron injection and charge recombination.
通过密度泛函计算，探索了基于三苯胺的染料敏化 TiO2 太阳能电池超快电子注入的合理机制以及对锚定基团的功率转换效率的显著依赖性。计算表明，染料敏化 TiO2 体系表面陷阱态的超快电荷复合可归因于带罗丹宁基的 A3 染料的羧基缺少电子密度。预测的 A1-3 吸附 TiO2 体系的电子和光学性质表明，直接电子注入源于染料 HOMO-1 到 TiO2 导带底的电子激发。在此基础上，对染料及其吸附体系相关前线轨道和能带的电子密度分布进行了讨论，这些分布在电子注入和电荷复合中起着重要作用。
