Mechanisms of positron annihilation on molecules

The aim of this work is to identify the mechanisms responsible for very large rates and other peculiarities observed in low-energy positron annihilation on molecules. The two mechanisms considered are: (i) Direct annihilation of the incoming positron with one of the molecular electrons. This mechanism dominates for atoms and small molecules. I show that its contribution to the annihilation rate can be related to the positron elastic scattering cross section. This mechanism is characterized by strong energy dependence of the annihilation rate at small positron energies if a low-lying virtual level or a weakly bound state exists for the positron. (ii) Resonant annihilation, which takes place when the positron undergoes resonant capture into a vibrationally excited quasibound state of the positron-molecule complex. This mechanism dominates for larger molecules capable of forming bound states with the positron. For this mechanism the energy-averaged annihilation rate is proportional to the level density of the positron-molecule complex, which is basically determined by the spectrum of molecular vibrational states populated in the positron capture. For room-temperature positrons this mechnism can produce annihilation rates up to 5 orders of magnitude greater than the first one. Its contribution is inversely proportional to the positron momentum at small positron energies.Comment: 28 pages, 5 figures, REVTeX, scheduled for publication in Phys. Rev. A, Feb 200

γ\gamma-ray spectra and enhancement factors for positron annihilation spectra with core-electrons

Many-body theory is developed to calculate the $\gamma$-spectra for positron annihilation with valence and core electrons in the noble gas atoms. A proper inclusion of correlation effects and core annihilation provides for an accurate description of the measured spectra [Iwata \textit{et al.}, Phys. Rev. Lett. {\bf 79}, 39 (1997)]. The theory enables us to calculate the enhancement factors $\gamma_{nl}$, which describe the effect of electron-positron correlations for annihilation on individual electron orbitals $nl$. We find that the enhancement factors scale with the orbital ionization energy $I_{nl}$ (in electron-volt), as $\gamma_{nl}=1+\sqrt{A/I_{nl}}+(B/I_{nl})^{\beta}$, where $A\approx 40$~eV, $B\approx 24$~eV and $\beta\approx 2.3$.Comment: 5 pages, 5 figure

Effect of dipole polarizability on positron binding by strongly polar molecules

A model for positron binding to polar molecules is considered by combining the dipole potential outside the molecule with a strongly repulsive core of a given radius. Using existing experimental data on binding energies leads to unphysically small core radii for all of the molecules studied. This suggests that electron-positron correlations neglected in the simple model play a large role in determining the binding energy. We account for these by including polarization potential via perturbation theory and non-perturbatively. The perturbative model makes reliable predictions of binding energies for a range of polar organic molecules and hydrogen cyanide. The model also agrees with the linear dependence of the binding energies on the polarizability inferred from the experimental data [Danielson et al 2009 J. Phys. B: At. Mol. Opt. Phys. 42 235203]. The effective core radii, however, remain unphysically small for most molecules. Treating molecular polarization non-perturbatively leads to physically meaningful core radii for all of the molecules studied and enables even more accurate predictions of binding energies to be made for nearly all of the molecules considered.Comment: 26 pages, 18 figure

Many-body theory calculations of positron binding to negative ions

A many-body theory approach developed by the authors [Phys. Rev. A 70, 032720 (2004)] is applied to positron bound states and annihilation rates in atomic systems. Within the formalism, full account of virtual positronium (Ps) formation is made by summing the electron-positron ladder diagram series, thus enabling the theory to include all important many-body correlation effects in the positron problem. Numerical calculations have been performed for positron bound states with the hydrogen and halogen negative ions, also known as Ps hydride and Ps halides. The Ps binding energies of 1.118, 2.718, 2.245, 1.873 and 1.393 eV and annihilation rates of 2.544, 2.482, 1.984, 1.913 and 1.809 ns$^{-1}$, have been obtained for PsH, PsF, PsCl, PsBr and PsI, respectively.Comment: 19 pages, 13 figures, submitted to International Review of Atomic and Molecular Physic

Ps-atom scattering at low energies

A pseudopotential for positronium-atom interaction, based on electron-atom and positron-atom phase shifts, is constructed, and the phase shifts for Ps-Kr and Ps-Ar scattering are calculated. This approach allows us to extend the Ps-atom cross sections, obtained previously in the impulse approximation [Phys. Rev. Lett. 112, 243201 (2014)], to energies below the Ps ionization threshold. Although experimental data are not available in this low-energy region, our results describe well the tendency of the measured cross sections to drop with decreasing velocity at $v<1$ a.u. Our results show that the effect of the Ps-atom van der Waals interaction is weak compared to the polarization interaction in electron-atom and positron-atom scattering. As a result, the Ps scattering length for both Ar and Kr is positive, and the Ramsauer-Townsend minimum is not observed for Ps scattering from these targets. This makes Ps scattering quite different from electron scattering in the low-energy region, in contrast to the intermediate energy range from the Ps ionization threshold up to $v\sim 2$ a.u., where the two are similar.Comment: 26 pages, 10 figure

Similarity between positronium-atom and electron-atom scattering

We employ the impulse approximation for description of positronium-atom scattering. Our analysis and calculations of Ps-Kr and Ps-Ar collisions provide theoretical explanation of the similarity between the cross sections for positronium scattering and electron scattering for a range of atomic and molecular targets observed by S. J. Brawley et al. [Science 330, 789 (2010)].Comment: 10 pages, 3 figure

Multiphoton detachment from negative ions: new theory vs experiment

In this paper we compare the results of our adiabatic theory (Gribakin and Kuchiev, Phys. Rev. A, accepted for publication) with other theoretical and experimental results, mostly for halogen negative ions. The theory is based on the Keldysh approach. It shows that the multiphoton detachment rates and the corresponding n-photon detachment cross sections depend only on the asymptotic behaviour of the bound state radial wave function. The dependence on the exponent is very strong. This is the main reason for the disagreement with some previous calculations, which employed bound state wave functions with incorrect asymptotic forms. In a number of cases our theoretical results produces best agreement with absolute and relative experimental data.Comment: 9 pages, Latex, IOP style, and 3 figures fig1.ps, fig2.ps, fig3.ps, submitted to J. Phys.

Calculations of positron binding and annihilation in polyatomic molecules

A model-potential approach to calculating positron-molecule binding energies and annihilation rates is developed. Unlike existing ab initio calculations, which have mostly been applied to strongly polar molecules, the present methodology can be applied to both strongly polar and weakly polar or nonpolar systems. The electrostatic potential of the molecule is calculated at the Hartree-Fock level, and a model potential that describes short-range correlations and long-range polarization of the electron cloud by the positron is then added. The Schrodinger equation for a positron moving in this effective potential is solved to obtain the binding energy. The model potential contains a single adjustable parameter for each type of atom present in the molecule. The wave function of the positron bound state may be used to compute the rate of electron-positron annihilation from the bound state. As a first application, we investigate positron binding and annihilation for the hydrogen cyanide (HCN) molecule. Results for the binding energy are found to be in accord with existing calculations, and we predict the rate of annihilation from the bound state to be $\Gamma=0.1$--$0.2 \times 10^9~\text{s}^{-1}$.Comment: 13 pages, 6 figures, accepted by J. Chem. Phy