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Polarization in Strong-Field Ionization of Excited Helium

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 Publication date 2021
  fields Physics
and research's language is English




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We analyze how bound-state excitation, electron exchange and the residual binding potential influence above-threshold ionization (ATI) in Helium prepared in an excited $p$ state, oriented parallel and perpendicular to a linearly polarized mid-IR field. Using ab initio B-spline Algebraic Diagrammatic Construction (ADC), and several one-electron methods with effective potentials, including the Schrodinger solver Qprop, modifi



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The orientation-dependent strong-field ionization of CO molecules is investigated using the fully propagated three-dimensional time-dependent Hartree-Fock theory. The full ionization results are in good agreement with recent experiments. The comparisons between the full method and single active orbital (SAO) method show that although the core electrons are generally more tightly bounded and contribute little to the total ionization yields, their dynamics cannot be ignored, which effectively modify the behaviors of electrons in the highest occupied molecular orbital. By incorporating it into the SAO method, we identify that the dynamic core polarization plays an important role in the strong-field tunneling ionization of CO molecules, which is helpful for future development of tunneling ionization theory of molecules beyond single active electron approximation.
Attosecond pump-probe ionization process can be used to prepare atomic ions in the coherent superposition of states with opposite parity. The multiphoton shake-up ionization of Helium, in particular, generates ions with same principal quantum number and a net dipole moment that evolves on a time scale of few picoseconds, due to spin-orbit coupling. In this work we use an ab initio time-dependent close-coupling code to study how the coherence between levels of Helium ion can be controlled from the parameters of the ionizing-pulse sequence. The observed periodic revivals, on a picosecond time scale, of the ion dipole moment gives access to the study of the ionization of oriented targets.
Strong-field ionization of atoms by circularly polarized femtosecond laser pulses produces a donut-shaped electron momentum distribution. Within the dipole approximation this distribution is symmetric with respect to the polarization plane. The magnetic component of the light field is known to shift this distribution forward. Here, we show that this magnetic non-dipole effect is not the only non-dipole effect in strong-field ionization. We find that an electric non-dipole effect arises that is due to the position dependence of the electric field and which can be understood in analogy to the Doppler effect. This electric non-dipole effect manifests as an increase of the radius of the donut-shaped photoelectron momentum distribution for forward-directed momenta and as a decrease of this radius for backwards-directed electrons. We present experimental data showing this fingerprint of the electric non-dipole effect and compare our findings with a classical model and quantum calculations.
Strong-field ionization and rescattering beyond the long-wavelength limit of the dipole approximation is studied with elliptically polarized mid-IR pulses. We have measured the full three-dimensional photoelectron momentum distributions (3D PMDs) with velocity map imaging and tomographic reconstruction. The ellipticity-dependent 3D-PMD measurements revealed an unexpected sharp, thin line-shaped ridge structure in the polarization plane for low momentum photoelectrons. With classical trajectory Monte Carlo (CTMC) simulations and analytical methods we identified the associated ionization dynamics for this sharp ridge to be due to Coulomb focusing of slow recollisions of electrons with a momentum approaching zero. This ridge is another example of the many different ways how the Coulomb field of the parent ion influences the different parts of the momentum space of the ionized electron wave packet. Building on this new understanding of the PMD, we extend our studies on the role played by the magnetic field component of the laser beam when operating beyond the long-wavelength limit of the dipole approximation. In this regime, we find that the PMD exhibits an ellipticity-dependent asymmetry along the beam propagation direction: the peak of the projection of the PMD onto the beam propagation axis is shifted from negative to positive values with increasing ellipticity. This turnover occurs rapidly once the ellipticity exceeds $sim$0.1. We identify the sharp, thin line-shaped ridge structure in the polarization plane as the origin of the ellipticity-dependent PMD asymmetry in the beam propagation direction. These results yield fundamental insights into strong-field ionization processes, and should increase the precision of the emerging applications relying on this technique, including time-resolved holography and molecular imaging.
221 - K. Fehre , S. Eckart , M. Kunitski 2020
We investigate the differential ionization probability of chiral molecules in the strong field regime as a function of the helicity of the incident light. To this end, we analyze the fourfold ionization of bromochlorofluoromethane (CHBrClF) with subsequent fragmentation into four charged fragments and different dissociation channels of the singly ionized methyloxirane. We observe a variation of the differential ionization probability in a range of several percent. Accordingly, we conclude that the helicity of light is a quantity that should be considered for the theoretical description of the strong field ionization rate of chiral molecules.
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