Multielectron wave-packet propagation for the investigation and manipulation of charge-migration processes and thereby emitted radiation

近年来，激光泵浦探测实验技术的飞速发展，使得对各种超快过程进行亚飞秒分辨率的直接实时观测成为可能。这为研究在核动力学开始发挥作用之前在阿秒/飞秒时间尺度上发生的过程打开了大门。因此，像内壳电子激发后电子系统重排这样的过程现在可以在时间和空间上进行追踪和分析。如果激发态的能量足够高，系统也可以经历非辐射衰变，并且外层价电子将从原子结合中逃脱。同时，为了正确地解释实验结果，人们需要精确的从头计算来提供电子云的时间演化，考虑到各种效应，如电子相关和电子弛豫。我们的项目致力于开发一种多电子波包传播的计算方法，使我们能够在考虑系统中所有电子的情况下，从头开始描述各种去激发过程的动力学。我们计划实时研究不同的衰变过程，以及外部激光脉冲对过程动力学的影响。所提出的理论研究结果将对解释和指导未来的实验研究至关重要。

In recent years, the tremendous development of laser pump-probe experimental techniques made possible a direct observation in real time of different kinds of ultrafast processes with sub-femtosecond resolution. This opened the door for investigation of processes in the attosecond/femtosecond time scale that take place before the nuclear dynamics comes to play. Thus, processes like the rearrangement of the electronic system following an excitation of an inner-shell electron can now be traced in time and space and analyzed. If the energy of the excited state is sufficiently high the system can also undergo a non- radiative decay and an outer-valence electron will escape from the atomic binding. In the same time, in order to interpret properly the experimental results, one needs precise ab initio calculations which provide the time evolution of the electronic cloud, taking into account various effects, as electronic correlation and electronic relaxation. Our project is devoted to the development of a computational methodology for multielectron wave- packet propagation giving the possibility to describe fully ab initio the dynamics of various de-excitation processes taking into account all electrons of the system. We plan to study in real time different decay processes, as well as the influence of an external laser pulse on the dynamics of the processes. The results of the proposed theoretical research will be essential for interpreting and guiding future experimental studies.