强场电离分子激发态非绝热过程原子核与电子动力学的理论研究

强激光场中分子的电离动力学和激发态非绝热动力学均为超快超强激光物理领域备受关注的研究热点。然而，由于同时考虑原子核和光电子的运动理论研究十分困难，因而关于这两种动力学过程共同发生的理论研究工作进展缓慢。本项目探索性地在表面跳跃方法之中引入蒙特卡洛波包方案模拟分子电离过程的技术路线，结合这两种方法的优势，可以实现对电子和原子核运动行为的量子力学描述。项目以不同激光参数下电离双原子分子的激发态非绝热动力学过程为研究内容，致力于得到不同反应通道下原子核和光电子的关联能谱，利用能谱结构特征提取激发态寿命、电子相干时间等重要信息，揭示非绝热相互作用对电子和原子核耦合运动行为的影响规律，进而阐明分子激发态原子核与电子的相互作用机制。项目研究成果可实现对分子内原子核或电子动力学行为的复现与控制，为精确调控分子反应动力学提供理论支撑。

Both the ionization dynamics and the non-adiabatic excitation dynamics in molecules driven by ultra-intense and ultrashort laser pulses have become two of the most popular research topics in the field of ultrafast and ultrastrong laser physics. However, there have been very few advances in developing new theoretical methods to study the coupled excitation and ionization dynamics because of the great difficulty of considering the quantum effects for both the nuclei and photoelectrons. In this project, we propose a new method of introducing the technical routes of the Monte Carlo wave packet method into the Surface Hopping method to realize a quantum mechanical description of both the electron and nuclear dynamics by combining the advantages of these two methods. We will apply it to study the non-adiabatic excited-state dynamics following ionization of different diatomic molecules by using ultrashort laser pulses at different laser parameters and to extract information such as the lifetime of excited states and the electronic coherence time from the obtained electron-nuclear coincidence energy spectra. The results from this work will help to reproduce and control the electron and nuclear dynamics in molecules, and thus provide a theoretical basis for a more precise control over the molecular reaction dynamics.