Ion-atom Collisions Research Articles

Experimental subshell vacancies in a multiply ionised Sn atom by heavy ion impact

The adoption of Heavy Ion PIXE for elemental quantification remains limited by the lack of fundamental atomic parameters needed for the calculation of X-ray production cross section data. Widely adapted theoretical models used for approximating ionisation cross sections, as well as other atomic physical parameters such as X-ray fluorescence yields, are calculated based on single-hole vacancy production post ion-atom impact. This renders the use of conventional ‘protonic’ models invalid for heavy ion-atom collisions. The degree to which Multiple Ionisation (MI) manifests in different heavy ion-atom collision symmetries significantly modifies atomic physical parameters. This is due to the significant number of introduced spectator vacancies in higher subshells, especially where near-symmetry is approached and MI is more pronounced. Knowledge of the mean number of vacancies in upper subshells is thus important for modifying atomic parameters that are needed for the translation of ionisation to X-ray production cross sections. In the present study, MI effects for Sn L-shell X-rays were studied using characteristic X-ray energy shifts measured using a standard PIXE spectrometer induced by Si, Cu and I projectile ions with incident energies up to 0.75 MeV/u. MI satellite distributions were studied using a Wavelength dispersive X-ray spectrometer (WDS) for high resolution PIXE, induced by C and Si projectile ions with incident ion energies up to 1.25 MeV/u. The mean number of subshell vacancies in the M- and N- shell for energy shifted Sn Lα X-ray lines were determined using both standard and high resolution PIXE spectrometers.

Multiple differential electron spectra from detachment in collisions of 30–300-keV anions with atoms and molecules

We have measured triple differential momentum distributions for electron detachment in collisions of 30- and 300-keV anions (C− and Si−) with atoms and molecules (He, Ar, and N2). The entire angular range of the ejected electrons was covered. The binary encounter ring, well known from positive ion-atom collisions, was observed in most cases. In a quasifree-electron scattering model this structure represents elastic scattering of the active electron from the target. However, especially for the slowest projectiles, this model fails to reproduce the angular distributions. In this regime it is probably necessary to use quasimolecular models to describe the collision. Indications for a projectile cusp are observed, implying that excitation-induced dipole moments in the ion projectile may be important. Published by the American Physical Society 2024

Gas-phase hydrogenation processes of cationic carbon clusters

ABSTRACT In this work, the gas-phase ion–atom collision reaction between large cationic carbon clusters and H-atoms is investigated. The carbon cluster cations (C$_{48-2*n}$$^+$, n = [0$-$8]) are produced from the photo-fragmentation processes of large PAH (dicoronylene, DC, C$_{48}$H$_{20}$) cations. The hydrogenated carbon cluster cations are efficiently formed (e.g. C$_{44/46}$H$_{9}$$^+$), and no even–odd hydrogenated mass patterns are observed. The hydrogenation behaviour and hydrogenation rate for these carbon cluster cations are the same. With theoretical calculations, the formation and bending processes of carbon cluster cations, the structure of these newly formed hydrogenated carbon cluster cations, and the bonding energies for the hydrogenation pathways are investigated. During the formation process of carbon clusters, the zigzagged edges gradually increase, and the planar configuration tends towards a bent and folded molecular configuration, i.e. from graphene to fullerene structures. The bending process with higher exothermic energies provides a reasonable explanation for the formation of the ‘magic numbers’ (e.g. C-atoms = 44) carbon clusters and their greater stability. The exothermic energy for each hydrogenation reaction pathway is relatively high; consequently, the forms and the hydrogenated states of carbon clusters are complex. The hydrogenation ability of edge carbon sites is higher than that of internal carbon sites; after bending and folding, the hydrogenation ability of these originally internal carbon sites becomes higher due to structural caged. As a result, under the co-evolution interstellar chemistry network, the (hydrogenation) states and forms of carbon compounds are complicated and diverse in the ISM.

Ruling out a saddle-point mechanism of ionization in intermediate-energy ion-atom collisions

Ruling out a saddle-point mechanism of ionization in intermediate-energy ion-atom collisions

Development of a cylindrical mirror analyser electron spectrometer and associated data acquisition system to study inner shell electron emission following ion-atom collision

In this paper we report on the development and performance of a cylindrical mirror analyser electron spectrometer for ion atom collision experiments. A low cost data acquisition system using Arduino microcontroller has also been developed and tested. We have measured the Auger emission spectra for various gaseous targets in collision with 1 MeV proton beams. Relative total Auger emission cross sections have also been measured for N2 molecular target as a function of incident proton energy. The projectile energy dependence agrees well with earlier reported measurements.

Time-Dependent Density Functional Theory for Atomic Collisions: A Progress Report

In this paper, the current status of time-dependent density functional theory (TDDFT)-based calculations for ion–atom collision problems is reviewed. Most if not all reported calculations rely on the semiclassical approximation of heavy particle collision physics and the time-dependent Kohn–Sham (TDKS) scheme for computing the electronic density of the system. According to the foundational Runge–Gross theorem, all information available about the electronic many-body system is encoded in the density; however, in practice it is often not known how to extract it without resorting to modelling and approximations. This is in addition to a necessarily approximate implementation of the TDKS scheme due to the lack of precise knowledge about the potential that drives the equations. Notwithstanding these limitations, an impressive body of work has been accumulated over the past few decades. A sample of the results obtained for various collision systems is discussed here, in addition to the formal underpinnings and theoretical and practical challenges of the application of TDDFT to atomic collision problems, which are expounded in mostly nontechnical terms. Open problems and potential future directions are outlined as well.

A high resolution reaction microscope with universal two-region time-focusing method.

This paper presents a novel reaction microscope designed for ion-atom collision investigations, established at the Institute of Modern Physics, Chinese Academy of Sciences, Lanzhou, China. Its time-of-flight (TOF) spectrometer employs an innovative flight-time focusing method consisting of two acceleration regions, providing optimal time focusing conditions for charged fragments with diverse initial velocities. The TOF spectrometer's axis intentionally tilts by 12° relative to the ion beam direction, preventing potential obstructions from the TOF grid electrodes. The introduced focusing method allows for a flexible time-focusing TOF spectrometer design without restricting the length ratio of the two regions. In addition, this configuration in our case significantly suppresses noise on the recoil ion detector produced by residual gas in the ion beam trajectory, which is a considerable challenge in longitudinal spectrometers. In a test experiment on the single electron capture reaction involving 62.5 keV/u He2+ ions and a helium atomic beam, the recoil longitudinal momentum resolution achieved 0.068 atomic units. This novel configuration and successful test run show excellent precision for ion-atom collision studies.

A Critical Analysis of Target Ionization and Projectile Electron Loss in Neutral– and Ion–Atom Collisions

Electron removal (target ionization and/or projectile electron loss) in neutral–atom collisions is theoretically studied for the impact of H0, He0 and He+ beams on noble gases (He, Ne and Ar). These reactions are investigated theoretically within the Continuum Distorted Wave-Eikonal Initial State model. New features have been included in the theoretical model: (i) a scaled projectile charge depending on its velocity and charge, (ii) a dynamic projectile-effective-charge depending on the momentum transfer, and (iii) a dynamic target-effective-charge depending on the kinematics of the emitted electron. The energy and angular spectra of emitted electrons from the target and from the projectile are calculated and compared with the available experimental data. Also, the influence of each one of the corrections on the resulting spectra will be studied.

Various mechanisms for double capture from helium targets by alpha particles

An analysis is presented using six quantum-mechanical four-body distorted wave (DW) theories for double capture (DC) in ion-atom collisions at intermediate and high energies. They all satisfy the correct boundary conditions in the entrance and exit channels. This implies the usage of short-range perturbation potentials in compliance with the exact behaviors of scattering wave functions at infinitely large separations of particles. Specifically, total cross sections Q are analyzed for collisions of alpha particles with helium targets. Regarding the relative quantitative performance of the studied DW theories at different impact energies E, our main focus is on the sensitivity of Q to various collisional mechanisms. The usual mechanism in most DW theories assumes that both electrons undergo the same type of collisions with nuclei. These are either single or double collisions in one or two steps, respectively, per channel, but without their mixture in either channel. The signatures of double collisions in differential cross sections are the Thomas peaks. By definition, these cannot be produced by single collisions. There is another DC pathway, which is actually favored by the existing experimental data. It is a hybrid, two-center mechanism which, in each channel separately, combines a single collision for one electron with a double collision for the other electron. The ensuing DW theory is called the four-body single-double scattering (SDS-4B) method. It appears that this mechanism in the SDS-4B method is more probable than double collisions for each electron in both channels predicted by the four-body continuum distorted wave (CDW-4B) method. This is presently demonstrated for Q at energies E=[200,8000] keV in DC exemplified by alpha particles colliding with helium targets.

Gas Phase Hydrogenated and Deuterated Fullerene Cations

H/D accretion, especially onto ionized fullerenes, is expected to be very efficient in space. In this work, we study hydrogenated and deuterated fullerene cations and their photodissociation behavior in the gas phase. The experimental results show that hydrogenated fullerene cations (i.e., [C60H n ]+ and [C70H n ]+, n up to 30) and deuterated fullerene cations (i.e., [C60D n ]+ and [C70D n ]+, n up to 21) are formed efficiently through the ion-atom collision reaction pathway. Upon irradiation, the hydrogenated and deuterated fullerene cations dissociate into fullerene cations and H/H2 or D/D2 species. The structures of the newly formed hydrogenated and deuterated fullerene cations (C58 and C60) and the bonding energies for these reaction pathways are investigated by means of quantum chemical calculations. The competition between hydrogenation and dehydrogenation is confirmed, and the hydrogenation-to-dehydrogenation ratio in the accretion processes in the gas phase is determined. We infer that the proportion of accreted hydrogen and deuterium atoms on the surface of fullerenes is similar to that of hydrogen and deuterium atoms in the interstellar environment where these fullerenes are located, especially when the interstellar environments are similar to our experimental conditions, i.e., the hot environment.

Dynamic effective charge in the continuum of the CDW-EIS model for ionization in ion–atom collisions: angular and energy dependence

In this work, a dynamic charge is employed in the continuum distorted wave–eikonal initial state theoretical model to describe the non-Coulomb potential of the residual target for single ionization in bare ion–multielectron atom collisions. A comparison between the well-known Belkić prescription and the effective charge depending on emission angle and energy in the final residual-target continuum state is shown. The obtained results show that this effective charge improves the description of double-differential cross sections for backward emission angles over the whole emission energy range allowing the calculation of simple differential and total cross sections.

Impact ionization of highly charged ion-atom collisions considering strong magnetic field and plasma screening effect

The impact ionization process of target is a crucial issue in the study of Heavy Ion Beam (HIB)-driven Magnetized Inertial Fusion (MIF). The collision systems between heavy projectile ions (Xeq+, Biq+, Uq+) and light target atoms/ions (H, D, T, 3He, 3He+, 11B) are promising candidate reactions for fusion power. In this study, the impact ionization process in medium-energy (ranges 1–100 MeV/u) is studied numerically based on the extended Classical-trajectory Monte Carlo (CTMC) method, where the effects of projectile charge state, external magnetic field and plasma screening on the single ionization process are considered. The results show that the existed external magnetic field results in a decrease of the yield of ionized high-energy electrons, whereas the yield of backward emitted electrons is increased. The effect of plasma screening on the ionization process is shown to be determined by the competition between the screening charge of projectile ion and the target nucleus. Thus, a significant decrease of ionization cross section is found in the low energy region since the screening charge of projectile ion is dominant. However, the screening effect of target nucleus charge is dominant in high energy region, where a significant increase of ionization cross sections is found.

Photon angular distribution of radiative electron capture into high-Z projectiles: A brief review

With the revolutionary development in the design of heavy-ion cooler storage rings and detectors, increasing interest is being focused on ion-atom collisions, in which the projectiles with a velocity comparable to the speed of light and the electronic transitions in inner shells of high-[Formula: see text] ions are involved. For this purpose, a fundamental interaction mechanism between a photon and an atomic electron in the presence of a strong Coulomb field is reviewed from the perspective of radiative electron capture into highly-charged ions. This is followed by the discussions of photon-electron interactions beyond the dipole approximation, which can be unambiguously visible in the photon angular distributions. In addition, the interference between the leading electric dipole transition [Formula: see text] and the magnetic multipole transition [Formula: see text] for the case of Lyman-[Formula: see text] radiation in hydrogen-like projectiles is also discussed.

Target polarization effect on energy loss of O<sup>5+</sup> ions near Bohr velocity in low density hydrogen plasma

Energy loss of ions near the Bohr velocity in plasma is one of the important topics in intense heavy ion beam driven high energy density physics and inertial confinement fusion. Based on the ions-plasma interaction experimental platform at HIRFL, this work shows the new experimental energy loss results of 1.07 MeV (~66.9 keV/u) O<sup>5+</sup> ions penetrating through a low-density partially ionized hydrogen plasma target (radio frequency plasma). The decrease of energy loss with free electron density increasing is found, which is very different from our previous result. The new experimental results are discussed by considering the theoretical models which involves the charge screening of projectiles in the partially ionized plasma and the target polarization effect-Barkas correction term. For the charge screening , the comparison between the momentum transfer under the Coulomb potential and that under the Debye potential is given, but due to the low ionization degree, the plasma screening effect seems not to be the main reason for the decrease of energy loss. For the target polarization effect , in the Bohr velocity regime, the Barkas correction term can play a key role in the ion-atom collisions. Modeling the Barkas correction term based on the proposed classical energy loss formula, the experimental data of ions in the gas target can be well fitted by the calculated values. In the partially ionized plasma, the frequent thermal electron collisions can give rise to the atomic excitation of plasma target, correspondingly the Barkas correction term changes: it decreases with the fraction of excited atoms increasing. As a result, the energy loss decreases in our experiment. In the stopping of highly charged ions in a partially ionized low-density plasma, the collisions between ions and free electrons can produce an enhanced energy loss according to previous studies. However, the target polarization effect, especially the atomic excitations, can significantly reduce the energy loss, which is observed in our experiment. Therefore, the interaction between ions and partially ionized plasma should be further studied, and the Barkas correction can be a very important term.

Analysis and simulation of time-of-flight spectrum in Rb<sup>+</sup>-Rb hybrid trap

The time-of-flight mass spectrum of charged particles, which are created through two-step cw-laser photoionization of laser-cooled <sup>87</sup>Rb atoms in an ion-neutral hybrid trap, is quantitatively investigated to further facilitate the study of Rb<sup>+</sup>-Rb reactive collisions. A microchannel plate (MCP) is used to detect charged particles, and two spectral peaks corresponding to the <sup>87</sup>Rb<sup>+</sup> ions and the product <inline-formula><tex-math id="Z-20230423060254-1">\begin{document}$ \rm {}^{87}Rb_2^+ $\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="9-20222273_Z-20230423060254-1.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="9-20222273_Z-20230423060254-1.png"/></alternatives></inline-formula> of the Rb<sup>+</sup>-Rb reaction were observed in the time-of-flight spectrum, respectively. The two peaks overlapped with each other and both showed an asymmetric profile. The information about the intensity, position, and half-width of the peak for a specific ion species was derived by fitting the time-of-flight spectrum with the probability density function of the Gumbel distribution. Then the relative ion intensity was converted into absolute ion number through the following steps. The rate equation of the total number of ions, which includes the number of atoms, the calibration factor of MCP, and the effective decay rate of ions in the ion trap, was established by modeling the photoionization of atoms. Combined with the absolute number of atoms measured by absorption imaging, the calibration factor in converting the ion intensity into the ion number was derived and the relative ion intensity was converted into the absolute number of ions. This provides a method of calibrating the MCP. The reliability of our calibration method was proved by the fact that the calibration factor in converting the intensity measured by MCP into particle number is independent of the duration of photoionization, the intensity and wavelength of the ionizing laser. Moreover, in order to explain the relationship between the peak width and temperature of the corresponding ion species, the time-of-flight spectra of the ions trapped in the ion trap were simulated by using COMSOL Multiphysics. The simulation results demonstrated that the large ion kinetic energy results in a narrow spectral peak. In sum, we quantitatively analyze and simulate the time-of-flight spectrum of the photoionization of cold atoms in the Rb<sup>+</sup>-Rb hybrid trap. The absolute number of ions is obtained by the intensity of the spectral peak, and the width of the spectral peak is related to the temperature of the ions. These results lay a foundation for the in-depth analysis of the ion-atom reaction collision and charged particle temperature relaxation in the photoionization of cold atoms, and thus further elucidating the subsequent collisional dynamics of ultracold plasmas.

High-energy two-electron transfer in ion-atom collisions

Two-electron transfer by fast heavy nuclei from heliumlike targets is studied. A detailed sequence of comprehensive computations is carried out in a large keV–MeV range of the projectile energies. This set is illustrated with total cross sections for double capture by alpha particles from helium atoms using several frequently applied four-body quantum-mechanical distorted wave models with the correct boundary conditions. The sensitivity of the obtained total cross sections is examined for different choices of the bound and continuum states. Especially at high energies, the influence of the compactness of the bound states is investigated by reference to the mechanism of the velocity matching kinematic double electron capture. Also considered is the dependence of these cross sections on the electronic screening of the projectile and the target nuclear charges in the bound and continuum states. The impact of this electronic shielding on total cross sections is assessed by reference to the corresponding bare nuclear charges in the bound and continuum states. Relative to all the available experimental data (100–6000 keV), the found striking model-dependence implies that two-electron transfer is sharply different from the associated one-electron transfer involving the same colliding particles.

Coherent treatment of transfer-excitation processes in swift ion-atom collisions

For more than 40 years since the first ion-atom collision investigations of the two-electron process of electron transfer with excitation and its resonant and nonresonant features, a satisfactory quantum mechanical treatment has been lacking. We present now such a comprehensive transfer excitation treatment using a three-electron atomic orbital close-coupling approach within a full configuration interaction formalism, exemplified by ${\mathrm{C}}^{4+}(1{s}^{2})+\mathrm{He}$ collisions at 0.5--18 MeV impact energies. The calculated cross sections for the production of ${\mathrm{C}}^{3+}(1s2{p}^{2}\phantom{\rule{0.16em}{0ex}}^{2}D)$, which shows the strongest resonance signature among the KLL Auger transitions, are found to be in excellent agreement with zero-degree Auger projectile spectroscopy measurements covering the maximum of the resonance peak and its high energy wing. At the lower energies, the theoretical results show a second maximum which is interpreted through a nonresonant one-step transfer excitation mechanism, never considered to date. The present, fully coherent, many-body treatment provides an important advance in the modeling and understanding of multielectronic processes in quantum systems under strong and ultrafast perturbations.

Double hyperbolic cosine basis sets for LCAO calculations

Recently, we reported a new set of hyperbolic cosine type basis sets, which include the radial part of exponential type functions. In this study, it is show that the double hyperbolic cosine basis sets with non-integer Slater type orbitals give extremely accurate results, with the accuracy superior to that of the previous similar calculations. Total energy differences and comparison between double hyperbolic cosine and other similar basis sets suggested in literature are presented. Using double hyperbolic cosine orbitals, combined Hartree–Fock-Roothaan calculations have been carried out on the ground states of atoms and their ions within the minimal basis sets framework to compare the performance of the basis sets. The basis sets achieved the accuracy far beyond the double-zeta quality. Proposed basis sets can also play an effective role in ion-atom collisions problems and semi-empirical methods.

Homonuclear ion-atom collisions: Application toLi+−Li

We present a theoretical framework for homonuclear, ground-state ion-atom collisions wherein the indistinguishability of direct elastic and resonant charge exchange (RCE) scattering channels is discussed. The discussion in terms of the total cross section(${\ensuremath{\sigma}}_{\text{tot}}$) is motivated and derived. The standard cross-section expressions for direct elastic(${\stackrel{\ifmmode \tilde{}\else \~{}\fi{}}{\ensuremath{\sigma}}}_{\text{el}}$) and RCE (${\stackrel{\ifmmode \tilde{}\else \~{}\fi{}}{\ensuremath{\sigma}}}_{\text{ce}}$) channels are obtained as high-energy approximations to ${\ensuremath{\sigma}}_{\text{tot}}$. We show that the total cross section resolves the inconsistency, at low energies, between the diffusion cross section (${\ensuremath{\sigma}}_{D}$) and the high-energy approximation to the total cross section (${\stackrel{\ifmmode \tilde{}\else \~{}\fi{}}{\ensuremath{\sigma}}}_{\text{tot}}$). The validity of the equivalence relation between the ${\ensuremath{\sigma}}_{D}$ and $2\ifmmode\times\else\texttimes\fi{}{\stackrel{\ifmmode \tilde{}\else \~{}\fi{}}{\ensuremath{\sigma}}}_{\text{ce}}$ is also discussed. The differences which result in cross sections which are frequently used in the description of ion-atom collision is illustrated with specific calculations for an ${\mathrm{Li}}^{+}\ensuremath{-}\mathrm{Li}$ system. The use of ${\ensuremath{\sigma}}_{\text{tot}}$ is advocated as a correct and consistent way to represent cross sections.

Non-Relativistic Electronic-Structure Computation of Neutral and Cationic Systems [Fr2, Fr-AEM+ (AEM= Ca, Sr, Ba)

The experimental field of ultracold ion-atom mixtures including an alkali-metal atom and an alkaline-earth-metal ion as well as of homonuclear alkali dimers has paved the way for creating and manipulating the ultracold molecules. The present paper is focused on a study of molecules such us francium dimer and a comparative spectroscopic investigation of the cationic systems Fr-(Ca+, Sr+, Ba+). We adopt a computational scheme without spin-orbit coupling reposed on the full configuration interaction and semi-empirical pseudo-potential theory of the atomic cores Fr+, Ca2+, Sr2+, and Ba2+ with extended and optimized basis sets. We have determined the adiabatic potentials with their relative spectroscopic constants, the electric dipole moments and the vibrational levels spacings for the 1,3Σu,g+ and 1,3Σ+ electronic states for Fr2 and Fr-AEM+, respectively, correlated toward {Fr(7s) + Fr(7s, 7p, 6d, 8s, 8p)}, {Ca(4s2, 4s4p, 4s3d), Sr(5s2, 5s5p, 5s4d), Ba(6s2, 6s6p, 6s5d) + Fr+}, and {Ca+(4s, 3d), Sr+(5s, 4d), Ba+(6s, 5d) + Fr(7s, 7p)}. The accuracy and reliability of the current results are discussed by comparing with theoretical data available in the literature. The occurrence of some avoided crossings between the neighboring electronic states is leading to a charge or excitation transfer for atom-ion collisions in the diverse charge or excited states. The Σ+-Σ+ transitions are determined in order to evaluate the future radiative lifetimes of vibrational states serving the direct laser cooling.