It is generally believed that the recollision mechanism of atomic nonsequential double ionization is suppressed in circularly polarized laser fields because the returning electron is unlikely to encounter the core. On the contrary, we find that recollision can and does significantly enhance double ionization, even to the extent of forming a ``knee,'' the signature of the nonsequential process. Using a classical model, we explain two apparently contradictory experiments, the absence of a knee for helium and its presence for magnesium.
14 August 2017 in The Journal of Physical Chemistry Letters
We identify the phase-space structures that regulate atomic double ionization in strong ultrashort laser pulses. The emerging dynamical picture complements the recollision scenario by clarifying the distinct roles played by the recolliding and core electrons, and leads to verifiable predictions on the characteristic features of the “knee”, a hallmark of the nonsequential process.
5 May 2016 in Journal of Physics B: Atomic, Molecular and Optical Physics
We investigate the process of circularly polarized high harmonic generation in molecules using a bicircular laser field. In this context, we show that molecules offer a very robust framework for the production of circularly polarized harmonics, provided their symmetry is compatible with that of the laser field. Using a discrete time-dependent symmetry analysis, we show how all the features (harmonic order and polarization) of spectra can be explained and predicted. The symmetry analysis is generic and can easily be applied to other target and/or field configurations.
First-principles calculations are employed to elucidate the modes of attosecond charge migration (CM) in halogenated hydrocarbon chains. We use constrained density functional theory (DFT) to emulate the creation of a localized hole on the halogen and follow the subsequent dynamics via time-dependent DFT. We find low-frequency CM modes () that propagate across the molecule and study their dependence on length, bond order, and halogenation. We observe that the CM speed () is largely independent of molecule length, but is lower for triple-bonded versus double-bonded molecules. Additionally, as the halogen mass increases, the hole travels in a more particlelike manner as it moves across the molecule. These heuristics will be useful in identifying molecules and optimal CM detection methods for future experiments, especially for halogenated hydrocarbons which are promising targets for ionization-triggered CM.
We show that a family of key periodic orbits drives the recollision process in a strong circularly polarized laser field. These orbits, coined recolliding periodic orbits, exist for a wide range of parameters, and their relative influence changes as the laser and atomic parameters are varied. We find the necessary conditions for recollision-driven nonsequential double ionization to occur. The outlined mechanism is universal in that it applies equally well beyond atoms: The internal structure of the target species plays a minor role in the recollision process.