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arXiv:1712.00842 · Physical Review A

Quantum coherent control of the photoelectron angular distribution in bichromatic-field ionization of atomic neon

Грызлова Елена Владимировна, Alexei N. Grum-Grzhimailo, Ekaterina I. Staroselskaya, Nicolas Douguet, Klaus Bartschat

Published Jan 26, 2018• 29 citations
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Abstract

We investigate the coherent control of the photoelectron angular distribution in bichromatic atomic ionization. Neon is selected as target since it is one of the most popular systems in current gas-phase experiments with free-electron lasers (FELSs). In particular, we tackle practical questions, such as the role of the fine-structure splitting, the pulse length, and the intensity. Time-dependent and stationary perturbation theory are employed, and we also solve the time-dependent Schr\"odinger equation in a single-active electron model. We consider neon ionized by a FEL pulse whose fundamental frequency is in resonance with either $2p\text{\ensuremath{-}}3s$ or $2p\text{\ensuremath{-}}4s$ excitation. The contribution of the nonresonant two-photon process and its potential constructive or destructive role for quantum coherent control is investigated.

DOI
10.1103/physreva.97.013420

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We investigate the coherent control of the photoelectron angular distribution in bichromatic atomic ionization. Neon is selected as target since it is one of the most popular systems in current gas-phase experiments with free-electron lasers (FELSs). In particular, we tackle practical questions, such as the role of the fine-structure splitting, the pulse length, and the intensity. Time-dependent and stationary perturbation theory are employed, and we also solve the time-dependent Schr"odinger equation in a single-active electron model. We consider neon ionized by a FEL pulse whose fundamental frequency is in resonance with either 2p\ensuremath-3s2p\text{\ensuremath{-}}3s2p\ensuremath-3s or 2p\ensuremath-4s2p\text{\ensuremath{-}}4s2p\ensuremath-4s excitation. The contribution of the nonresonant two-photon process and its potential constructive or destructive role for quantum coherent control is investigated.
Coherent control of the photoelectron angular distribution (PAD) in ionization by a bichromatic circularly polarized field is theoretically studied in neon in the photon energy range 16--20 eV. The breakdown of the PAD axial symmetry with respect to the light propagation direction is analyzed. The coherent control of the PAD manifests itself through: (1) a change from a one-lobe to a three-lobe shape, respectively, for co- and counter-rotating harmonics, (2) a variation of the polar asymmetry with the light frequency, and (3) a rotation of the PAD around the direction of the beam depending on the relative phase between the harmonics. Tuning the lowest harmonic at the 2p53s2{p}^{5}3s2p53s or 2p54s2{p}^{5}4s2p54s intermediate excited states strongly influences the PAD. In contrast to atomic hydrogen and the alkali atoms, the cases of equal and opposite helicity are not related in neon. Features of a conjugate polarization setup, when one harmonic is linearly polarized while the other one is circularly polarized, are also discussed.
We investigate the coherent control of nonresonant two-photon excitation and (2+12+12+1) photon ionization processes from the time-dependent perspective. To this end, we have solved the time-dependent Schr\"odinger equation for a hydrogen atom interacting with an ultraviolet laser field. Results are obtained for symmetric and antisymmetric phase distributions leading to dark and bright pulses, for which the temporal field distributions consist of many subpulses. For the two-photon excitation process, it is found that at intermediate time between the subpulses, the population in the excited state can exceed the final state population and, in particular, is nonzero for dark pulses. The results for the (2+12+12+1) photon ionization closely follow those for the excitation process, which shows that the ionization of the electron proceeds as a resonant process via the excited state in all cases considered.
Abstract We investigate features of electron emission from atoms in the field of the fundamental and second harmonic of a laser in conditions relevant to those realized in free-electron lasers. General expressions for the angular anisotropy and photoelectron spin polarization are obtained. These expressions are used for describing of the ionization of the valence shell of inert gas atoms and illustrated by calculations for neon. The possibility of control over the electron emission characteristics by varying the relative phase between harmonic (i.e., realization of one of the forms of the coherent control) is considered.
We present first-principles numerical simulations of photoionization in neon induced by bichromatic extreme ultraviolet pulses with frequencies ωωω and 2ω2ω2ω, specially chosen to make ωωω equal to the energy difference between the 2s2s2s and 2p2p2p subshells. This allows for the production of photoelectrons from the 2s2s2s shell by 2ω2ω2ω pulse and from the 2p2p2p shell by ωωω pulse with the same energy. Using the multi-configurational time-dependent Hartree-Fock method, we explore how Rabi coupling between subshells generates coherence between the corresponding photoelectron wave packets. Our \textit{ab initio} calculations confirm the analytical results derived from the essential-states approach in [K. L. Ishikawa, K. C. Prince, and K. Ueda, J. Phys. Chem. A 127, 10638 (2023)], validating the theoretical predictions. Although we focus on the Ne 2p2p2p and 2s2s2s subshells, our approach is applicable to a broad range of systems exhibiting photoionization from multiple subshells. The laser parameters employed in our simulations are available in modern Free Electron Lasers (FELs), and we anticipate that this work could stimulate experimental investigations using FELs to study ion-photoelectron coherence and entanglement.
In the paper we present the angular distributions of photoelectrons in ionization of neon atom by a field of several multiple frequencies. The considered setup is refered to the RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) spectroscopy under condition that the field frequencies are selected in such a way that resonant transitions through discrete states play an important role. The role of the phase of the seed infrared field on the angular distributions of photoemission is analyzed. A significant difference in the anisotropy parameters at the near-threshold sideband caused by transitions through discrete states is shown. Two methods are compared: numerical solution of rate equations with continuum discretization and third-order perturbation theory.