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Laser-induced electron diffraction (LIED), in which elastic scattering of the returning electron with the parent ion takes place, has been used to extract atomic potential and image molecular structures with sub-Å precision and exposure time of a few femtoseconds. So far, the polarization and exchange effects have not been taken into account in the theoretical calculation of differential cross section (DCS) for the laser-induced rescattering processes. However, the validity of this theoretical treatment has never been verified. In this work, we investigate the polarization and exchange effects on electron impact elastic scattering with rare gas atoms and ions. It is found that, while the exchange effect generally plays a more important role than the polarization effect in the elastic scattering process, the exchange effect is less important on electron–ion collisions than on electron–atom collisions, especially for scattering in backward direction. In addition, our calculations show that, for electron–atom collisions at incident energies above 50 eV, both the polarization and exchange effects can be safely neglected, while for electron–ion collisions, both the polarization and exchange potentials do not make substantial contributions to the DCS at incident energies above 20 eV and scattering angles larger than 90°. Our investigation confirms the validity of the current LIED method.
Collisions of electrons with atoms and ions are the basic physical processes that provide a unique diagnostic probe of the fundamental interactions in many-electron systems. While elastic scattering of electrons from neutral atoms has been extensively studied both experimentally and theoretically, experimental difficulties have limited the investigations on elastic scattering of electrons from ions. So far, measurements of cross sections for electron elastic scattering in free-electron ion collisions have been scarce. However, in recent years, there has been a large amount of experimental data available for differential cross section (DCS) of elastic scattering of electrons with singly charged atomic ions[1–5] as well as molecular ions.[6] These experimental DCSs were extracted from the measured two-dimensional (2D) momentum distributions for high energy photoelectrons in high-order above threshold ionization (HATI) based on the quantitative rescattering (QRS) model (see Ref. [7] and references therein).
The main philosophy of the QRS model is that the yields of laser-induced rescattering processes, which comprise elastic scattering, excitation, ionization, and recombination of the returning electron with the parent ion, can be expressed as a product of the returning electron wave packet (RWP) with various field-free electron–ion scattering cross sections. Among all the laser-induced rescattering processes, HATI is the simplest one in which the electron–ion elastic collision takes place. According to the QRS model, the 2D momentum distributions for high energy photoelectrons in HATI can be factorized as the RWP and the laser-free electron–ion elastic scattering DCS. It has been well documented that the RWP which can be evaluated from the second-order strong field approximation[8] depends only on the laser parameters. Owing to this property of the RWP, one is able to remove the laser’s influence and thus obtains the electron–ion elastic collision DCSs at large scattering angles from 100° to 180° and in a wide range of incident energy from the experimentally measured laser-induced electron diffraction (LIED) momentum distributions.
LIED has attracted wide interests in strong laser physics since it was first proposed to serve as a new tool to probe ultrafast molecular dynamics by Zuo et al.[9] two decades ago. It has been demonstrated that LIED can be used to extract the atomic potential[10] and to probe the detailed information about the electronic orbital and the position of the nuclei in molecules.[11] Furthermore, LIED has also been applied to molecular imaging with sub Å precision and exposure time of a few femtoseconds.[6] To our knowledge, in the theoretical treatment of LIED, the polarization and exchange effects have never been taken into account in the DCS calculations for electron–ion elastic scattering. However, since the incident electron influences the charge distribution of the target, an electric dipole is induced in the target during the collision, and the magnitude of the induced dipole depends on the polarizability. In the meantime, the scattering electron can potentially exchange with any of the bound electrons in the target. It has been well recognized that the effects of the charge cloud polarization in the target and exchange of the scattering electrons with the bound electrons are important in electron scattering from atoms, ions, and molecules, especially for low collision energies.
According to the semiclassical rescattering model,[12,13] in the LIED, one of the bound electrons that is first tunnel ionized near the peak of the laser’s oscillating electric field is subsequently driven by the laser field and has the chance to return back to the parent ion when the field changes direction, and then serves as an incident electron colliding with the parent ion. The maximum kinetic energy that a returning electron can gain from the field is 3.17 Up, where Up is the electron ponderomotive energy, which is proportional to the laser intensity. For a typical laser pulse with a wavelength of 800 nm and a peak intensity of
In this paper, we examine the energy dependence of the polarization and exchange effects in elastic scattering of electron with atoms and ions. The goal of the present work is to verify the validity of the current theoretical treatment of electron–ion elastic scattering in LIED.
Atomic units
We consider elastic scattering of electrons with Ne and Ar atoms as well as Ar+ ion, and employ the standard potential scattering theory to evaluate the elastic scattering DCSs. The details of the standard potential scattering theory have been presented in our previous paper.[14] Here only the scattering potentials used in the numerical calculations are given.
The static potential
The effect of polarization on the projectile can be modeled by adding a polarization potential to the static potential. Here we take the polarization potential to be of the Buckingham type[16]
The polarization potential given in Eq. (
In Eq. (
While the exchange potential for rare gas atoms can be determined with no ambiguity, the choice of the exchange potential for ions is somehow arbitrary. Firstly, there exists an ambiguity in the total spin of the two exchanging electrons. Although the total spin for the exchange of the projectile electron with one of the closed shell electrons in the target ion remains triplet, it is not clear if the projectile electron exchanges with an open shell electron, since in this case the total spin could be either triplet or singlet. Secondly, there are many different ways to construct the exchange potential. In this paper, we employ three different models for the local exchange potential which have been proposed originally for the exchange of the ejected electron with a bound electron in the residual ion in the process of electron impact ionization of Ar,[20] equivalent to the exchange of the projectile electron in elastic scattering by Ar+. The first model for the exchange potential for elastic scattering from an open shell ion is taken to be the same as that for elastic scattering from a closed shell atom, as given by Eq. (
We have performed theoretical calculations of the DCSs for elastic scattering of electrons by Ne and Ar atoms as well as Ar+ ion. We aim to investigate the energy dependence of the polarization and exchange effects on elastic scattering of electron with atoms and ions. Although the theoretical model employed in this paper is the same as that used by Nahar and Wadehra,[16] the separate quantitative contributions to the DCSs from the polarization and exchange potentials were not presented in Ref. [16]. Here, to demonstrate the effects of the charge cloud polarization in the target and exchange of the projectile electron with the bound electron, the DCSs by using the static potential only (“s”), the static potential plus local polarization potential (“sp”), the static potential plus local exchange potential (“se”), and the static potential with both local polarization and exchange potentials (“spe”) are calculated separately. It should be noted that in the “se” calculations, Vd in Eq. (
In Fig.
The polarization and exchange effects are expected to decrease with the increase of energy, as demonstrated in Figs.
Figure
In Fig.
In the theoretical calculations for the elastic scattering of electrons by Ar, the static potential completely fails to predict the double-dip structure in the DCSs observed in experiment for incident energies below 20 eV, and so does the static plus polarization potential, although obvious differences exist between the “s” and “sp” results. The agreement between theory and experiment is greatly improved if the exchange potential is included since, at least, the dip in the backward direction is well reproduced by the “se” calculations. As a matter of fact, the minima in both the forward and the backward directions can be reproduced by the static plus exchange potential for incident energies above 10 eV. Again, this indicates that the exchange potential is more important than the polarization potential.
For both Ne and Ar, as demonstrated in Figs.
It should be noted that the “spe” DCSs depend on the parameter d in Eq. (
Recall that the ultimate goal of the present work is to test the significance of the polarization and exchange effects in LIED in which the laser-induced electron scattering with the parent ions is treated as laser–free electron scattering with the target ions. For traditional scattering processes, experimental measurements of cross sections at backward angles up to 180° are typically formidable due to the mechanical constraints of the electron spectrometer. In LIED, on the contrary, only the backward scattering cross sections can be extracted from the HATI photoelectron momentum distributions, in which the elastic scattering cross sections in the forward directions are imbedded in the signal of direct ionization and hence are inaccessible. The backward scattering cross sections generally carry more structure information of the targets due to the fact that large angle scattering results from collisions with small impact parameters such that the electron probes the effective potential distribution inside the electron cloud of the target. Consequently, a more sophisticated theoretical description is required.
For elastic scattering of electrons with ions, the difficulty is associated with how to deal with the exchange between the projectile electron and an open shell electron. As discussed in the above section, there exists an ambiguity in the description of the exchange potential in local approximation. Following the prescriptions of Biava et al.,[20] here, we also try three different models for the LE potential, namely, LET, LE1, and LE5, for elastic scattering of electrons by Ar+. The success or failure of a LE potential should be decided by whether or not, and to what extent, using such a potential improves the agreement between the experimental data and the calculated results based on a no-exchange model. Biava et al.[20] have examined the accuracy of the LE potential for electron impact ionization of the p-shell electron of Ar and found that the LE approximation is reliable for ionization leading to s-state vacancies but not p-state vacancies.
In Fig.
To examine the accuracy of the three LE models, in Fig.
The comparison shown in Fig.
In Fig.
The effects of the polarization and exchange potentials are demonstrated in Fig.
We have investigated the polarization and exchange effects on elastic scattering of electrons with atoms and ions. Numerical calculations of differential cross sections based on the standard potential scattering theory have been performed for elastic scattering of electrons by Ne and Ar at incident energies from 5 eV to 100 eV, and by Ar+ at 3.3 eV and 16 eV. By including both the polarization and exchange potentials, the present theoretical results are in very good agreement with experiment for all the cases considered in the present paper, except for electron–Ar+ collision at 3.3 eV. Even for electron–Ar+ collision at 3.3 eV, the present “spe” DCSs are also very close to the R-matrix calculations.
The present numerical calculations agree with the well-known general trend that the polarization and exchange effects are very significant at low energies but become weaker as the energy increases. It has been found that, for elastic scattering of electrons with neutral atoms, both the polarization and exchange effects can be safely neglected for incident energies higher than 50 eV. Comparison of the theoretical results with the experimental data also reveals that the exchange potential plays a more important role than the polarization potential. Whereas, although it is more difficult to deal with the exchange between the projectile electron and the bound electron in an open shell, it has been found that the exchange effect is less important on electron–ion collisions than on electron–atom collisions, especially for scattering in the backward direction, provided that a proper local exchange potential is used. In the meanwhile, the polarization of ions is also depressed since the charge distribution of the core is more tightened compared to that of atoms.
In conclusion, for elastic scattering, both the polarization and exchange effects on electron–ion collisions are not as important as those on electron–atom collisions. Since only slight differences exist between the “s” and “spe” calculated DCSs for elastic scattering of electrons by Ar+ at 16 eV, it is reasonable to deduce that both the polarization and exchange effects can be ignorable for elastic electron–ion collisions at energies above 20 eV. This indicates that the current theoretical treatment of LIED is valid.
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