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Journal of Experimental and Theoretical Physics

Ionization of Atoms by a Bichromatic Fields of ω + 2ω Multiple Frequencies with Arbitrary Polarization

Maria M. Popova, Грызлова Елена Владимировна, Maksim D. Kiselev, Alexei N. Grum-Grzhimailo

Published Jul 1, 2022• 5 citations
Publisher

Abstract

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.

DOI
10.1134/s1063776122070044

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Spin polarization of photoelectrons is considered in the ionization of atoms by a laser field and its second harmonic, concentrating on the effects of interference between the two ionization paths. The possibility for a crucial increase of the spin polarization by manipulating the relative phase of the harmonics is demonstrated. Observation of these effects, exemplified by the ionization of neon atoms, is accessible by modern free-electron lasers working in the extreme-ultraviolet wavelength regime.
Abstract The biharmonic (ω, 2ω) photoionization of atomic inner-shell electrons opens up new perspectives for studying nonlinear light–atom interactions at intensities in the transition regime from weak to strong-field physics. In particular, the control of the frequency and polarization of biharmonic beams enables one to carve the photoelectron angular distribution and to enhance the resolution of ionization measurements by the (simultaneous) absorption of photons. Apart from its quite obvious polarization dependence, the photoelectron angular distributions are sensitive also to the (relative) intensity, the phase difference and the temporal structure of the incoming beam components, both at resonant and nonresonant frequencies. Here, we describe and analyze several characteristic features of biharmonic ionization in the framework of second-order perturbation theory and (so-called) ionization pathways, as they are readily derived from the interaction of inner-shell electrons with the electric-dipole field of the incident beam. We show how the photoelectron angular distribution and elliptical dichroism can be shaped in rather an unprecedented way by just tuning the properties of the biharmonic field. Since such fields are nowadays accessible from high-harmonic sources or free-electron lasers, these and further investigations might help extract photoionization amplitudes or the phase difference of incoming beams.
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.
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 consider electron scattering by hydrogen atoms in a bichromatic linearly polarized laser field of frequencies ω and 3ω and we discuss the coherent control of the scattering process as a function of the relative phase φ between the two components of the radiation field. The electrons are assumed to have sufficiently high energies in order to permit the description of the scattering process in the first-order Born approximation. The scattered electrons, embedded in the bichromatic laser field of moderate power, as well as the laser dressing of the hydrogen atoms in their ground state are described by time-dependent perturbation theory. We discuss the angular dependence of the nonlinear differential scattering cross sections for the low values N = ±2 of absorbed or emitted laser photons as a function of the relative phase φ between the two radiation field components. We also compare our results with those obtained from the assumption of a static potential describing the target atom.