为了研究四硫富瓦烯(TTF)基团对有机染料敏化剂光电性能的影响，以咔唑染料Dye 1为原型，引入TTF基团作为电子给体，设计了咔唑染料Dye 2.采用密度泛函理论(DFT)和含时密度泛函理论(TD-DFT)分别计算模拟了纯染料分子和吸附团簇(TiO2)9后的形貌、分子轨道能级以及紫外-可见吸收光谱，采用周期性密度泛函理论计算模拟染料分子在二氧化钛(101)面吸附的表面形貌.结果发现：在有机染料中引入TTF基团有助于有机染料敏化剂在二氧化钛表面的抗团聚作用和分子内的电荷转移；最为重要的是， TTF基团的强给电子能力极大地增强了有机染料敏化剂的光捕获能力.所有的计算结果表明， TTF基团是一种非常有潜力改善染料敏化剂光电性能的给电子基团.
To investigate the effect of a tetrathiafulvalene (TTF) unit on the photovoltaic properties of the corresponding dye sensitizer, a TTF-carbazole-based sensitizer, Dye 2, was designed;it was based on the framework of Dye 1. The geometries, electronic structures, and optical properties of Dye 1 and Dye 2 before and after binding to (TiO2)9 clusters were investigated using density functional theory (DFT) and time-dependent DFT. The surface morphologies of the dyes on TiO2 (101) surfaces were simulated by periodic DFT calculations using the DMol3 program. The calculated results showed that the introduction of TTF units into dyes could help to inhibit dye aggregation on the TiO2 surface; this is conducive to intramolecular charge-transfer transitions and significantly improves the light-harvesting ability. The calculated results demonstrate that the TTF unit is a very promising electron donor for improving the photovoltaic properties of organic dye sensitizers.
陈喜明;贾春阳;万中全;姚小军
电子科技大学微电子与固体电子学院，电子薄膜与集成器件国家重点实验室，成都610054兰州大学功能有机分子化学国家重点实验室，兰州730000
化学化工
四硫富瓦烯;染料敏化剂;密度泛函理论;含时密度泛函理论;染料敏化太阳能电池
Tetrathiafulvalene;Dye sensitizer;Density functional theory;Time-dependent density functional theory;Dye-sensitized solar cel
《物理化学学报》 2014 (002)
273-280 / 8
The project was supported by the National Natural Science Foundation of China (21272033), Innovation Fund of State Key Laboratory of Electronic Thin Films and Integrated Devices, China (CXJJ201104), and Beijing National Laboratory for Molecular Sciences, China (BNLMS)@@@@国家自然科学基金(21272033),电子薄膜与集成器件国家重点实验室创新基金(CXJJ201104)以及北京分子科学国家实验室(筹)开放基金资助项目
10.3866/PKU.WHXB201311262
评论