硅杂环戊二烯衍生物电子结构与光谱性质的理论研究

采用密度泛函理论(DFT)B3LYP/6-31G*方法, 对2,5位取代的硅杂环戊二烯(Silole)系列衍生物进行几何结构优化, 通过计算得到电离能、电子亲和势、空穴抽取能及电子抽取能等相关能量, 并使用TD-DFT方法研究其吸收光谱, 分析相关能量及光谱的变化规律. 采用单组态相互作用(CIS/6-31G*)方法优化得到它们的最低单重激发态(S1)结构, 在此基础上, 使用TD-DFT方法计算对应的发射光谱. 分析2,5位芳基取代硅杂环戊二烯衍生物(DADPS)激发态与基态的结构差异及原因, 研究前线分子轨道的分布情况, 并讨论发光特征及载流子传输性能. 研究结果表明, 激发态结构弛豫主要发生在Silole环和直接与2,5位芳基相连的部位; 前线轨道主要分布在Silole环和2,5位芳基上; 二吡咯取代物有望成为空穴传输材料, 二噻吩取代物和二呋喃取代物有望在发光器件中表现出较高的发光效率.

Theoretical Studies on the Electronic Structure and Spectra Properties of 1,1-Dimethyl-2,5-diaryl-3,4-diphenylsilole

The ground states and low-lying excited states of the four silole derivatives are fully optimized with the density functional theory-B3LYP and configuration interaction singles(CIS).On the basis of the geometries,we computed the ionization potentials(PI),electron affinities(EA),reorganization energies,and other energies.And we obtained the absorption and emission spectra with time-dependent density functional theory(TD-DFT) calculation on the ground states and excited states,respectively.The results for the four derivatives are studied in comparison to each other.Then we analyzed the varieties of the energies and the spectra,and explain that pyspy can act as electron injection material,and assign that the hole transfer material can be achieved based on prspr,finally point out that thsth and fusfu can act as emitting materials in bulk state.