Abstract
The attosecond ultrafast ionization dynamics of correlated two- or many-electron systems have, so far, been mainly addressed investigating atomic systems. In the case of single ionization, it is well known that electron–electron correlation modifies the ionization dynamics and observables beyond the single active electron picture, resulting in effects such as the Auger effect or shake-up/down and knock-up/down processes. Here, we extend these works by investigating the attosecond ionization of a molecular system involving correlated two-electron dynamics, as well as non-adiabatic nuclear dynamics. Employing a charge-transfer molecular model system with two differently bound electrons, a strongly and a weakly bound electron, we distinguish different pathways leading to ionization, be it direct ionization or ionization involving elastic and inelastic electron scattering processes. We find that different pathways result in a difference in the electronic population of the parent molecular ion, which, in turn, involves different subsequent (non-adiabatic) postionization dynamics on different time scales.
Highlights
For many elementary processes in multi-electron systems, such as in photoionization, electron-impact ionization, the Auger effect, and other radiative processes, the impact of correlated electron-electron dynamics plays a crucial role [1]
We extend these works by investigating the attosecond ionization of a molecular system involving correlated two-electron dynamics, as well as non-adiabatic nuclear dynamics
We find that different pathways result in a difference in the electronic population of the parent molecular ion, which, in turn, involves different subsequent postionization dynamics on different time scales
Summary
For many elementary processes in multi-electron systems, such as in photoionization, electron-impact ionization, the Auger effect, and other radiative processes, the impact of correlated electron-electron dynamics plays a crucial role [1]. The remaining bound electron(s) can be excited (shake-up/knockup processes [2]), relaxed (shake-down/knock-down), or even ejected subsequently (Auger process) [3]. Such time-resolved ionization dynamics of multi-electron systems have been investigated in various theoretical and experimental studies, for a review see for example Ref. 4. The advent of ultrashort femtoor even attosecond pulses in the extreme ultraviolet (XUV) regime being available either via table-top high-order harmonic generation or the newest generation of (X)FEL sources, for example, paved the way for the observation of these processes in real time, e.g. employing the attosecond streaking technology [5,6,7,8,9]. Resolving the details of these complex correlated many-body phenomena involving nuclear and electronic degrees of freedom still poses a challenge for computational simulations
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