Attosecond-pump attosecond-probe spectroscopy in non-equilibrium ensembles

要了解原子和分子的行为，需要了解组成这些系统的电子和原子核的动力学。这种动力学的典型时间尺度是飞秒(S 10-15)。我们需要使用比这更短的光脉冲来启动动力学，然后捕捉它。这种动力学是由量子相干驱动的。在这个项目中，我们将用新的计算例程来增强最先进的R-矩阵的时间依赖代码，以跟踪量子相干性。这将使我们能够将几个单独的计算合并为一个总体计算。这项工作将提供支持未来在世界领先的激光设备上进行阿秒泵浦阿秒探测器实验的能力，以及阐明泵浦激光诱导的量子动力学的能力。我们将把这种方法应用到涉及自由电子激光设备中的顺序电离的演示问题，包括外层电子和内层电子的发射。我们还研究了该方法预测特定动态的最优参数的能力。

Understanding how atoms and molecules behave requires understanding of the dynamics of electrons and nuclei that make up these systems. The typical timescale for this dynamics is the femtosecond (10-15 s). We need to use light pulses shorter than this to initiate the dynamics and then to capture it. The dynamics is driven by quantum coherence. In this project, we will enhance the state-of-the-art R-matrix with time dependence code with new computational routines to keep track of the quantum coherence. This will enable us to combine several individual calculations into one overarching calculation. This work will provide capability to support future attosecond-pump attosecond-probe experiments at world-leading laser facilities, and capability to elucidate quantum dynamics induced by the pump laser. We will apply the approach to demonstration problems involving sequential ionization at free-electron laser facilities involving the emission of both outer and inner-shell electrons. We also investigate the capability of the approach to predict optimal parameters for specific dynamics.