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Physica Scripta

On the Energy Dependence of Annihilation Cross-Sections for Positrons in Collision with Atoms and Molecules

Peter Van Reeth, Gaetana Laricchia, J W Humberston

Published Jan 1, 2005• 19 citations
Publisher

Abstract

The very large annihilation rates observed at room temperature in positron collisions with certain molecules have instigated the development of several models of positron annihilation based on the role of virtual processes, Feshbach resonances and bound states. One of the outcomes of these models has been the interest they have generated in investigations of the energy dependence of the annihilation cross-section in the vicinity of inelastic thresholds. The aim of this article is to provide a review of these recent studies and to highlight outstanding questions.

DOI
10.1238/physica.regular.071a000c9

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The very large annihilation rates observed at room temperature in positron collisions with certain molecules have instigated the development of several models of positron annihilation based on the role of virtual processes, Feshbach resonances and bound states. One of the outcomes of these models has been the interest they have generated in investigations of the energy dependence of the annihilation cross-section in the vicinity of inelastic thresholds. The aim of this article is to provide a review of these recent studies and to highlight outstanding questions.
Measurements of positron-on-molecule annihilation have established that positrons bind to a variety of molecules via vibrational Feshbach resonances. Data for deeply bound states in benzene and 1-chlorohexane and for positronically excited (i.e., second) bound states in alkanes are used to establish the dependence of annihilation rates on the binding energy and incident positron energy. With this dependence removed, annihilation rates for a broad class of molecules lie on a universal curve as a function of the number of molecular vibrational degrees of freedom. The implications of these results for theoretical models are discussed.
An overview is presented of recent studies of the interaction of low-energy positrons with atoms and molecules using a trap-based positron beam. The beam is tunable from ~100 meV to many electron volts, with a typical energy resolution of 25 meV (FWHM). A variety of scattering processes are investigated using the properties of positron orbits in a spatially varying magnetic field. Recent scattering measurements are reviewed, and new data for electronic excitation, ionization, and positronium formation in noble gases are presented. In a separate set of experiments, positron annihilation below the threshold for positronium formation is studied in molecules as a function of positron energy. The data show large Feshbach resonances in the range of energies of the molecular vibrations. Within the framework of this model, these results provide the first experimental evidence that positrons bind to hydrocarbon molecules.
Positron cooling and annihilation in room temperature noble gases is simulated using accurate scattering and annihilation cross sections calculated with many-body theory, enabling the first simultaneous probing of the energy dependence of the scattering and annihilation cross sections. A strikingly small fraction of positrons is shown to survive to thermalization: ∼0.1 in He, ∼0 in Ne, ∼0.15 in Ar, ∼0.05 in Kr, and ∼0.01 in Xe. For Xe, the time-varying annihilation rate Z[over ¯]_{eff}(τ) is shown to be highly sensitive to the depletion of the momentum distribution due to annihilation, conclusively explaining the long-standing discrepancy between gas-cell and trap-based measurements. Overall, the use of the accurate atomic data gives Z[over ¯]_{eff}(τ) in close agreement with experiment for all noble gases except Ne, the experiment for which is proffered to have suffered from incomplete knowledge of the fraction of positrons surviving to thermalization and/or the presence of impurities.
The present results report a computational analysis of the effects of symmetric bond stretching during positron scattering from polyatomic hydrocarbon molecules in the gas phase. The collisions are considered at very low energies where the behavior of the sss-wave scattering length can be analyzed and where signatures of virtual state formation appear for all the three systems considered (C2H2{\mathrm{C}}_{2}{\mathrm{H}}_{2}C2​H2​, C2H4{\mathrm{C}}_{2}{\mathrm{H}}_{4}C2​H4​, and C2H6{\mathrm{C}}_{2}{\mathrm{H}}_{6}C2​H6​). Furthermore, the present calculations show that the stretching of the CH bonds in all molecules causes the moving of the existing virtual state closer to threshold and further makes it become a bound state whenever highly distorted molecules are involved. The effects of these changes are further seen to cause a marked enhancing of the corresponding annihilation parameters Zeff{Z}_{\mathit{eff}}Zeff​ at low collision energies, in line with what is experimentally observed for such gases. The significance of such model calculations is discussed in some detail.
The elastic and annihilation cross sections for positron-cadmium scattering are reported up to the positronium-formation threshold (at 2.22.22.2 eV). The low-energy phase shifts for the elastic scattering of positrons from cadmium were derived from the bound and pseudostate energies of a very large basis configuration-interaction calculation of the e+{e}^{+}e+-Cd system. The sss-wave binding energy is estimated to be $126\ifmmode\pm\else\textpm\fi{}42$ meV, with a scattering length of ${A}_{\mathrm{scat}}=(14.2\ifmmode\pm\else\textpm\fi{}2.1)$a0{a}_{0}a0​, while the threshold annihilation parameter, Zeff{Z}_{\mathrm{eff}}Zeff​, was $93.9\ifmmode\pm\else\textpm\fi{}26.5$. The ppp-wave phase shift exhibits a weak shape resonance that results in a peak Zeff{Z}_{\mathrm{eff}}Zeff​ of $91\ifmmode\pm\else\textpm\fi{}17$ at a collision energy of about $490\ifmmode\pm\else\textpm\fi{}50$ meV.
A two-parameter semiempirical theory of positron scattering and annihilation is developed and used to investigate the behavior of positrons interacting with the rare gases and metal vapors. The two-parameter theory is able to do a reasonable job of reproducing existing cross section and annihilation data for the rare gases. A model-potential calculation that correctly predicts the behavior of the phase shifts will also predict the energy dependence of Zeff(k){Z}_{\mathrm{eff}}(k)Zeff​(k) even if the magnitude is incorrect. Analysis of the Zeff{Z}_{\mathrm{eff}}Zeff​ versus temperature data of Kurz et al. [Phys. Rev. Lett. 77, 2929 (1996)] suggests scattering lengths of $\ensuremath{-}5.6\ifmmode\pm\else\textpm\fi{}{1.0a}_{0},$ $\ensuremath{-}10.3\ifmmode\pm\else\textpm\fi{}{2.0a}_{0},$ and $\ensuremath{-}56\ifmmode\pm\else\textpm\fi{}{15a}_{0}$ for Ar, Kr, and Xe, respectively. Existing bound-state calculations can be used to fix the values of the semi-empirical parameters for a number of metal vapors, resulting in predicted Zeff{Z}_{\mathrm{eff}}Zeff​ of 119, 36, and 94 for Be, Mg, and Cu at threshold. In addition to the calculations, expressions relating the threshold form of Zeff(k){Z}_{\mathrm{eff}}(k)Zeff​(k) to the complex scattering length are presented.