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Physical Science International Journal

Phase and Ellipticity Dependence of the Photoelectron Angular Distribution in Non Resonant Three Photon Ionization of Atomic Hydrogen

Mamadou Faye

Published Jun 28, 2011• 0 citations
OpenAlex

Abstract

We studied the ellipticity and the dependence on the phase lag (lead) (between the semi major and the semi minor axes of the field components) of the photoelectron angular distribution (PAD) in the non resonant three photon ionization of atomic hydrogen. The exact analytical expressions for azimuthal PAD for 1s, 2s, 3s, 2p, 3p and 3d, initial states, are given.In comparison with dipole-dipole transitions, the number of quantum paths increases from: two to three for s-states; three to six for p-states; four to seven for d-states; while the number of angular coefficients goes from four to six, with two asymmetric terms. It is important that these asymmetric terms giving rise to the elliptic dichroism (ED), are only constituted with the imaginary part of the interference associated to the authorized channels leading to final states. Using the ED expression, we have established the phase shift isolation’s equation for l=0 instead of l=0,1, initial states, previously. Similarly, it is notable that, the submagnetic levels, m=0 for l=1; m=±1, for l=2, initial states, do not contribute to the PAD.Numerical evaluation of the angular coefficients is given for each state. The PAD shapes and the ED signals have been analyzed. It is found that, the maxima or the minima and the directions, of the PAD (1s, 2s, 3s, 3p), depend on the competing angular coefficients, which in return are affected by the interference terms. It is interesting to note that ,the asymmetric terms contribute only when the PAD maxima are shifted from the semi major or semi minor axes(2p,3d);and the isotropic shape(1s,2s,2p,3p,3d) is strongly dependent on the isotropic term. It is also observed that, when the photoelectron has a preference for the left handed or the right handed, the azimuthal detection difference between these two limit angles is reduced of one half than that obtained for dipole-dipole transitions. The highest ED signal (2p, 3p), occurs from the combination of the strong contributing asymmetric terms with the competing four first PAD terms. Besides, for 1s initial state, a nonzero ED signal is observed, at a particular value of the phase lag matching the phase shifts difference, for nearly circularly and nearly linearly polarized light.

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Phase and ellipticity dependence of the photoelectron angular distribution in non-resonant two-photon ionization of atomic hydrogen. I

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We study the ellipticity and the dependence on the phase lag (lead) (between the semimajor and the semiminor axes of the field components) of the photoelectron angular distribution (PAD) in the non-resonant two-photon ionization of atomic hydrogen. We establish exact analytical expressions for azimuthal PAD for 3s, 3p and 3d excited initial states, marked by the occurrence of an asymmetric term. This term gives rise to elliptic dichroism (ED), which can be obtained in two ways: either with the left (versus right) ellipticity, or with the phase lag (versus lead); for 3s and 3p initial states, it is shown that the quantum phase of continua is directly related to the phase lag, one-photon below-threshold ionization, and indirectly one photon above. Another important result is that the magnetic sublevels, m = 0, for 3p and m = ±1, for 3d, do not contribute to the azimuthal PAD. Our numerical results show, for 3s and 3d, and near-threshold ionization, that the PAD has maxima either along the semimajor or the semiminor axis, while for above-threshold ionization, they are always shifted from these axes. However, the maxima of the corresponding ED coincide with the PAD maxima, while for 3p, they are shifted from the PAD minima. A strong dependence of the ED sign is noted, regardless of the state or the process. However, strong ED signals are obtained for the 3s initial state and below-threshold ionization.

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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.

Physical Review A•Dec 12, 2019•15 citations
We studied the ellipticity and the dependence on the phase lag (lead) (between the semi major and the semi minor axes of the field components) of the photoelectron angular distribution (PAD) in the non resonant three photon ionization of atomic hydrogen. The exact analytical expressions for azimuthal PAD for 1s, 2s, 3s, 2p, 3p and 3d, initial states, are given.In comparison with dipole-dipole transitions, the number of quantum paths increases from: two to three for s-states; three to six for p-states; four to seven for d-states; while the number of angular coefficients goes from four to six, with two asymmetric terms. It is important that these asymmetric terms giving rise to the elliptic dichroism (ED), are only constituted with the imaginary part of the interference associated to the authorized channels leading to final states. Using the ED expression, we have established the phase shift isolation’s equation for l=0 instead of l=0,1, initial states, previously. Similarly, it is notable that, the submagnetic levels, m=0 for l=1; m=±1, for l=2, initial states, do not contribute to the PAD.Numerical evaluation of the angular coefficients is given for each state. The PAD shapes and the ED signals have been analyzed. It is found that, the maxima or the minima and the directions, of the PAD (1s, 2s, 3s, 3p), depend on the competing angular coefficients, which in return are affected by the interference terms. It is interesting to note that ,the asymmetric terms contribute only when the PAD maxima are shifted from the semi major or semi minor axes(2p,3d);and the isotropic shape(1s,2s,2p,3p,3d) is strongly dependent on the isotropic term. It is also observed that, when the photoelectron has a preference for the left handed or the right handed, the azimuthal detection difference between these two limit angles is reduced of one half than that obtained for dipole-dipole transitions. The highest ED signal (2p, 3p), occurs from the combination of the strong contributing asymmetric terms with the competing four first PAD terms. Besides, for 1s initial state, a nonzero ED signal is observed, at a particular value of the phase lag matching the phase shifts difference, for nearly circularly and nearly linearly polarized light.
We study the ellipticity and the dependence on the phase lag (lead) (between the semimajor and the semiminor axes of the field components) of the photoelectron angular distribution (PAD) in the non-resonant two-photon ionization of atomic hydrogen. We establish exact analytical expressions for azimuthal PAD for 3s, 3p and 3d excited initial states, marked by the occurrence of an asymmetric term. This term gives rise to elliptic dichroism (ED), which can be obtained in two ways: either with the left (versus right) ellipticity, or with the phase lag (versus lead); for 3s and 3p initial states, it is shown that the quantum phase of continua is directly related to the phase lag, one-photon below-threshold ionization, and indirectly one photon above. Another important result is that the magnetic sublevels, m = 0, for 3p and m = ±1, for 3d, do not contribute to the azimuthal PAD. Our numerical results show, for 3s and 3d, and near-threshold ionization, that the PAD has maxima either along the semimajor or the semiminor axis, while for above-threshold ionization, they are always shifted from these axes. However, the maxima of the corresponding ED coincide with the PAD maxima, while for 3p, they are shifted from the PAD minima. A strong dependence of the ED sign is noted, regardless of the state or the process. However, strong ED signals are obtained for the 3s initial state and below-threshold ionization.
Within the framework of second order time dependent perturbation theory and non relativistic dipole approximation, the exact expressions of the radial transition amplitude from 3d, 3p and 3s excited states, were obtained from the integral representation of the Green Coulomb function. Below threshold and above one photon ionization threshold, it can be expressed as an analytic combination of three Appell hypergeometric functions of first order, one of which is degenerated; while at threshold, it can be obtained in terms of an expansion of Gauss confluent hypergeometric functions. The angular coefficients are numerically evaluated and analysed for some available laser wavelengths.
We study in some detail the photoelectron angular distributions in two-colour three-photon ionization of the ground state hydrogen atom in its dependence on the polarizations of the two electromagnetic fields. We treat the particular case of photons propagating in the same direction and having elliptic polarizations with the same axes. The azimuthal distributions presented refer to the electrons emitted with momenta orthogonal to the photons direction. The calculations are done in nonrelativistic dipole approximation, in velocity gauge, using third-order perturbation theory. We show that the photoelectron azimuthal angular distributions have a fourfold symmetry only for identical linear or circular polarizations. In all the other cases the distribution has a twofold symmetry.
Within the framework of perturbation theory and of dipole approximation, the angular distribution for third order processes can be expressed for any state of quantum numbers (n, l) of the hydrogen atom as θθθ 642 coscoscos dcba +++; whatever the polarisation state (linear or circular). The explicit expressions of the corresponding angular coefficients are given for ns and np initial states. It is shown for the particular case of linear polarization that, the isotropic term a occurs only for initial states with orbital quantum number l greater than zero, and contains exactly twenty one contributing terms for np states; in the case of circularly polarized light, the distribution follows a sin6θ behaviour for ns states, while for np states, it is expressed as a combination of sin4θ and sin6θ. Using the implicit summation technique, nine radial transitions matrix elements are determined and a quantitative analysis of these coefficients is made for 1s, 2s, 3s, 2p and 3p initial states at various wavelengths, including the three photons ionization threshold; for linear polarization, the shapes are strongly dependent on both quantum numbers (n, l); while for circular polarization the shapes remain the same. Furthermore, the corresponding total cross sections obtained indirectly from these coefficients, are globally in agreement with that obtained directly from other methods.
The three-dimensional angular distribution of electrons in two-photon ionization of atoms by an elliptically polarized laser beam, from an initial state with arbitrary angular momentum J i , is expressed in terms of six frequency-dependent invariant atomic parameters. The specific effect of the field polarization on the angular distribution (the elliptic dichroism, ED) is discussed for the general case of elliptic polarization. The necessary conditions for a non-zero ED are established and its physical origin is explained. The general theory is illustrated by a simple analytical calculation for the -potential model. Numerical calculations of the angular distribution parameters for H and Cs atoms are also performed and the dependence of ED magnitude on the atomic quantum numbers and the photon frequency is discussed for different frequencies.
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.