Attosecond imaging and control of correlated electron dynamics in molecules

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Understanding dynamical processes often relies on our ability to resolve them in time. Advances in generating controlled few-cycle laser pulses and novel ultrashort XUV/Xray sources, from free electron laser (FEL)-based to attosecond high harmonic generation (HHG)-based, have opened completely new avenues for imaging electronic and nuclear dynamics in molecules, with applications in physics, chemistry and biology. The access to attosecond time scale may allow us to uncover the role of electron correlations in processes such as ultrafast charge migration, multiple ionization and autoionization in molecules, and address new fundamental questions about the role of attosecond coherent electron dynamics in chemical reactivity. We propose to study electronic and coupled electronic-nuclear dynamics in molecules at the attosecond to femtosecond time-scale, developing concepts and theoretical tools for interpreting new generation of ultrafast time-resolved experiments. We will develop a set of comprehensive theoretical approaches and tools for time-resolving and controlling (i) autoionization in the presence of ultra-fast vibrational motion, (ii) attosecond hole dynamics in molecules upon ionization, and (iii) coupled electronnuclear dynamics during non-adiabatic transitions, with emphasis on the role of electronic coherence created prior or during the transition.