飞秒时间分辨光电子影像对多原子分子非绝热动力学的研究

非绝热耦合在分子，特别是在多原子分子内部起着非常重要的作用，它控制着分子内部能量的分配和电荷的转移。由于非绝热耦合导致许多理论无法解释的现象，成为原子分子物理的一个研究重点。将飞秒泵浦/探测方法和光电子影像技术结合起来，形成飞秒时间分辨光电子影像（TRPEI）方法。该方法可以直接跟踪非稳定态（波包）的演变过程，利用它可以去详细研究分子内部的态态相互作用和态态间发生的非绝热耦合。本项目拟使用飞秒时间分辨的质谱、光离子和光电子影像方法，并结合波包传播理论研究芳香烃分子和杂环芳香烃分子的超快动力学,其中包括分子的电离解离过程，异构化和分子间电荷转移过程。研究重点在于分子超快过程所经历的非绝热耦合，主要集中于分子锥形交叉及其"channel three"区域动力学过程，期待能对多原子分子(主要是芳香烃分子)内部的非绝热耦合过程给出比较清晰的物理图像。

Non-adiabatic coupling, which dominant intra-molecular energy distribution and charge transfer in molecules, plays an important role in the intramolecular dynamics of molecular systems, especially in polyatomic molecules. Non-adiabatic coupling is a very important research priority in atomic and molecular physics because it leads to many phenomena which can't be explained by theories. Femtosecond time-resolved photoelectron imaging (TRPEI), which couples the femtosecond pump-probe and photoelectron imaging techniques, can real-time track the evolution of wave-packet directly and study the detailed intramolecular state-to-state interaction and non-adiabatic coupling. In this project, we plan to investigate the ultrafast dynamics of benzene derivatives and hetero-cyclic benzene derivatives using femtosecond time-resolved photoelectron and photoion imaging coupled with time-of-flight mass spectroscopy techniques. The key point is the non-adiabatic coupling involved in the ultrafast process of molecules, which including conical intersection(CI) and "channel three", in order to understand the nature of inter- and intra-molecular dynamics for benzene derivatives in detail.