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Physical Review A

Coherent control of the photoelectron angular distribution in ionization of neon by a circularly polarized bichromatic field in the resonance region

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

Published Dec 12, 2019• 15 citations

Abstract

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 $2{p}^{5}3s$ or $2{p}^{5}4s$ 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.

DOI: 10.1103/physreva.100.063417

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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

2{p}^{5}3s

or

2{p}^{5}4s

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.

A novel kind of coherent control of various atomic and molecular photoprocesses proceeding in a bichromatic electromagnetic (EM) laser field, angular coherent control , is proposed and demonstrated here theoretically by studying the particular case of negative-ion photodetachment in the field of a linearly polarized fundamental laser frequency and its second harmonic of arbitrary spatial configuration and orientation of the unit polarization vectors e 1 and e 2 of the respective harmonic fields. Due to the inherent spatial asymmetry of the applied bichromatic field, the ejection of detached photoelectrons is also generally asymmetric in respect of the detached photoelectron momentum replacement p →- p . As follows from our gauge-invariant analytical calculations within the framework of perturbation theory on EM interaction and a zero-range potential model for the negative ion, this field asymmetry results in a photocurrent, the magnitude and direction of which are strongly dependent on both the relative phase shift Φ between the harmonics of the ionizing bichromatic field and on the angle θ between the polarization vectors e 1 and e 2 . The latter strong dependence on the angle θ is the background for angular control of the direction and magnitude of the produced photocurrent by means of an appropriate choice and proper adjustment of the angle between the polarization vectors of the incident bichromatic field harmonics.

We investigate two-pathway interferences between nonresonant one-photon and resonant two-photon ionization of atomic hydrogen. In particular, we analyze in detail the photoionization mediated by the fundamental frequency and the second harmonic of a femtosecond VUV pulse when the fundamental is tuned near an intermediate atomic state. Following our recent study [Phys. Rev. A 91, 063418 (2015)] of such effects with linearly polarized light, we analyze a similar situation with circularly polarized radiation. As a consequence of the richer structure in circularly polarized light, characterized by its right-handed or left-handed helicity, we present and discuss various important features associated with the photoelectron angular distribution.

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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 $2p\text{\ensuremath{-}}3s$ 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.

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