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

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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.