R D Rivarola

Electron emission in heavy-ion-atom collisions

1. Introduction.- 2. Overview of Ionization Mechanisms.- 3. Theoretical Work.- 4. Experimental Methods.- 5. Ionization by Bare Projectiles.- 6. Ionization by Dressed Projectiles.- 7. Multiple Electron Processes.- 8. Concluding Remarks.- A. Summary of Analytic Cross Section Formulae.- B. Kinematic Effects on Electron Emission.- C. References to Double Differential Cross Section Studies.- References.

Two-centre effects in ionization by ion impact

When an atom is ionized by ion impact, the electron is ejected into a final continuum state of a two-centre potential due to the Coulomb fields of the projectile and ionized atom. The related effects on the electron yield or energy and angular distributions are referred to as two-centre electron emission (TCEE). The present report is devoted to a discussion of experimental and theoretical evidence of this TCEE. The use of heavy ions or antiprotons as projectiles allows to unravel these effects by monitoring the two centre potential. On the theoretical side, the continuum distorted wave-eikonal initial state theory (CDW-EIS) accounts for the TCEE thus allowing a detailed interpretation of the experimental findings.

A theoretical model for ionisation in ion-atom collisions. Application for the impact of multicharged projectiles on helium

The continuum-distorted-wave-eikonal-initial-state model is extended to describe single-electron ionisation by impact of bare projectiles on multielectronic targets. Applications are given for collisions between multicharged ions and helium. Double differential, single differential and total cross sections are calculated. Experimental data and present theoretical results show deviations from the square of the projectile charge dependence predicted by the first Born approximation.

A multi-scale ab initio theoretical study of the production of free radicals in swift ion tracks in liquid water

Using a multi-scale theoretical approach from first principles, we show that the production of HO2 radicals in liquid water can be understood from the initial Coulomb explosion of doubly ionized water molecules. Based on the separation of time scales, we used three different theoretical models, each one associated with a specific time scale. The initial ~1 fs of water radiolysis is taken care of with a Monte Carlo code whose basic ingredients are cross-sections. These have been calculated in the present work using the continuum distorted wave eikonal initial state (CDW-EIS) model framework. Our calculated cross-sections nicely demonstrate that double ionization of water molecules is one major event compatible with the experimental HO2 molecular rate production. The subsequent tens of fs following the double ionization of one water molecule of the liquid medium have been described with microscopic ab initio Car–Parrinello molecular dynamics simulations. Dynamics shows that the water Coulomb explosion leads to the formation of two H3O+ ions and an atomic oxygen atom. The final stage of the Coulomb explosion (up to the ms timescale) has been modelled with a chemical Monte Carlo code, assessing that the production of HO2 results from the O + OH → HO2 reaction in the liquid phase.

Quantum-mechanical predictions of DNA and RNA ionization by energetic proton beams

Among the numerous constituents of eukaryotic cells, the DNA macromolecule is considered as the most important critical target for radiation-induced damages. However, up to now ion-induced collisions on DNA components remain scarcely approached and theoretical support is still lacking for describing the main ionizing processes. In this context, we here report a theoretical description of the proton-induced ionization of the DNA and RNA bases as well as the sugar-phosphate backbone. Two different quantum-mechanical models are proposed: the first one based on a continuum distorted wave-eikonal initial state treatment and the second perturbative one developed within the first Born approximation with correct boundary conditions (CB1). Besides, the molecular structure information of the biological targets studied here was determined by ab initio calculations with the Gaussian 09 software at the restricted Hartree-Fock level of theory with geometry optimization. Doubly, singly differential and total ionization cross sections also provided by the two models were compared for a large range of incident and ejection energies and a very good agreement was observed for all the configurations investigated. Finally, in comparison with the rare experiment, we have noted a large underestimation of the total ionization cross sections of uracil impacted by 80 keV protons,whereas a very good agreement was shown with the recently reported ionization cross sections for protons on adenine, at both the differential and the total scale.

Theoretical predictions for ionization cross sections of DNA nucleobases impacted by light ions.

Induction of DNA double strand breaks after irradiation is considered of prime importance for producing radio-induced cellular death or injury. However, up to now ion-induced collisions on DNA bases remain essentially experimentally approached and a theoretical model for cross section calculation is still lacking. Under these conditions, we here propose a quantum mechanical description of the ionization process induced by light bare ions on DNA bases. Theoretical predictions in terms of differential and total cross sections for proton, α-particle and bare ion carbon beams impacting on adenine, cytosine, thymine and guanine bases are then reported in the 10 keV amu(-1)-10 MeV amu(-1) energy range. The calculations are performed within the first-order Born approximation (FBA) with biological targets described at the restricted Hartree-Fock level with geometry optimization. Comparisons to recent theoretical data for collisions between protons and cytosine point out huge discrepancies in terms of differential as well as total cross sections whereas very good agreement is shown with our previous classical predictions, especially at high impact energies (E(i) ≥ 100 keV amu(-1)). Finally, in comparison to the rare existing experimental data a systematic underestimation is observed in particular for adenine and thymine whereas a good agreement is reported for cytosine. Thus, further improvements appear as necessary, in particular by using higher order theories like the continuum-distorted-wave one in order to obtain a better understanding of the underlying physics involved in such ion-DNA reactions.

Proton-induced single electron capture on DNA/RNA bases.

In this work, we report total cross sections for the single electron capture process induced on DNA/RNA bases by high-energy protons. The calculations are performed within both the continuum distorted wave and the continuum distorted wave-eikonal initial state approximations. The biological targets are described within the framework of self-consistent methods based on the complete neglect of differential overlap model whose accuracy has first been checked for simpler bio-molecules such as water vapour. Furthermore, the multi-electronic problem investigated here is reduced to a mono-electronic one using a version of the independent electron approximation. Finally, the obtained theoretical predictions are confronted with the scarcely available experimental results.

Interference effects in single ionization of molecular hydrogen by electron impact

A recently developed molecular three-continuum approximation is employed to compute differential cross sections for the ionization of hydrogen molecules by electron impact. Within the framework of this approximation, the chosen final electronic wavefunction takes into account the molecular character of the target as well as the correlate motion between the aggregates in the final channel of the reaction. Fivefold-differential cross sections as a function of both the electron momenta in the final state and the molecular orientation are studied for different kinematical arrangements. Interference structures coming from the two-centre geometry of the molecule are predicted in this case. Integrated cross sections over all molecular orientations are also calculated. It is shown that interference patterns remain, even for this case.

Theoretical Calculation of Electronic Stopping Power of Water Vapor by Proton Impact

The energy loss of proton beams in water vapor is analyzed with a full quantum-mechanical treatment, the distorted-wave model. This model takes into account distortion effects due to the long-range Coulomb potential. Projectile energies from 10 keV up to 1 MeV are considered. Mean stopping power and equilibrium charge-state fractions are calculated and compared with experimental data. The validity of Braggs additivity rule is investigated.

Distorted wave theories for dressed-ion–atom collisions with GSZ projectile potentials

The continuum distorted wave and the continuum distorted wave-eikonal initial state approximations for electron emission in ion–atom collisions are generalized to the case of dressed projectiles. The interaction between the dressed projectile and the active electron is represented by the analytic Green–Sellin–Zachor (GSZ) potential. Doubly differential cross sections as a function of the emitted electron energy and angle are computed. The region of the binary encounter peak is analysed in detail. Interference structures appear in agreement with the experimental data and are interpreted as arising from the coherent interference between short- and long-range scattering amplitudes.