Maxwellianization of Positrons Cooling in CF_{4} and N_{2} Gases.

Positron cooling in CF_{4} and N_{2} gases via inelastic vibrational and rotational (de)excitations is simulated, importantly including elastic positron-positron collisions. For CF_{4}, it is shown that rotational (de)excitations play no role on the experimental timescale, and further, that in the absence of positron-positron collisions, cooling via excitation of the dipole-active ν_{3} and ν_{4} modes alone would lead to a non-Maxwellian positron momentum distribution, in contrast to the observations of experiment. It is shown that the observed Maxwellianization of the distribution may be effected by positron-positron collisions and/or cooling involving the combination of the dipole-inactive ν_{1} mode with the dipole-active modes. For N_{2}, rotational excitations alone are sufficient to Maxwellianize the distribution (vibrational effects are negligible).

Effect of molecular constitution and conformation on positron binding and annihilation in alkanes.

The model-potential approach previously developed by the authors to study positron interactions with molecules is used to calculate the positron binding energy for n-alkanes (CnH2n+2) and the corresponding cycloalkanes (CnH2n). For n-alkanes, the dependence of the binding energy on the conformation of the molecule is investigated, with more compact structures showing greater binding energies. As a result, thermally averaged binding energies for larger alkanes (n ≳ 9) show a strong temperature dependence in the range of 100 K-600 K. This suggests that positron resonant annihilation can be used as a probe of rotational (trans-gauche) isomerization of n-alkanes. In particular, the presence of different conformers leads to shifts and broadening of vibrational Feshbach resonances in the annihilation rate, as observed with a trap-based low-energy positron beam.

Positron Binding and Annihilation in Alkane Molecules.

A model-potential approach has been developed to study positron interactions with molecules. Binding energies and annihilation rates are calculated for positron bound states with a range of alkane molecules, including rings and isomers. The calculated binding energies are in good agreement with experimental data, and the existence of a second bound state for n-alkanes (C_{n}H_{2n+2}) with n≥12 is predicted in accord with experiment. The annihilation rate for the ground positron bound state scales linearly with the square root of the binding energy.

Many-Body Theory for Positronium-Atom Interactions.

A many-body-theory approach has been developed to study positronium-atom interactions. As first applications, we calculate the elastic scattering and momentum-transfer cross sections and the pickoff annihilation rate ^{1}Z_{eff} for Ps collisions with He and Ne. For He the cross section is in agreement with previous coupled-state calculations, while comparison with experiment for both atoms highlights discrepancies between various sets of measured data. In contrast, the calculated ^{1}Z_{eff} (0.13 and 0.26 for He and Ne, respectively) are in excellent agreement with the measured values.

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 Schrödinger 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 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 Γ = 0.1-0.2 × 109 s-1.

Vibrational Feshbach Resonances Mediated by Nondipole Positron-Molecule Interactions.

Measurements of energy-resolved positron-molecule annihilation show the existence of positron binding and vibrational Feshbach resonances. The existing theory describes this phenomenon successfully for the case of infrared-active vibrational modes that allow dipole coupling between the incident positron and the vibrational motion. Presented here are measurements of positron-molecule annihilation made using a recently developed cryogenic positron beam capable of significantly improved energy resolution. The results provide evidence of resonances associated with infrared-inactive vibrational modes, indicating that positron-molecule bound states may be populated by nondipole interactions. The anticipated ingredients for a theoretical description of such interactions are discussed.