The behavior of the Ps atom in molecular substances, particularly liquids, is investigated. The pickoff rates of o‐Ps in various liquid compounds are found to have a simple empirical relationship to the values of the surface tension of the liquids. The relationship is found to have a theoretical foundation. The Ps atom is highly localized in a cavity created by the balance of various molecular forces inside the liquid. From the above relationship, other simple relationships between the pickoff rates of o‐Ps and the various properties of the medium, e.g., polarizability, cohesive energy density, etc., and the temperature or pressure changes can be derived and explained. The diffusion of o‐Ps is discussed. A similar approach can also be used for molecular solids.

Positronium Annihilation in Molecular Substances

This review is concerned with the utilization of the positron-electron annihilation phenomenon in studies of the physics of condensed matter. The theory of the annihilation process is outlined, the importance of the two-photon mode of decay is established, and it is described how the observable results depend on the initial positron and electron states of the system. A brief account of the principal experimental techniques is included. Discussion of the complex nature of positron behavior in molecular substances suggests the particular value of investigations directed at the two photon pick-off mode of decay of the orthopositronium atoms that are formed in these materials. The possibility of positronium formation in ionic and metallic materials is also considered. The many important electron aspects of positron annihilation in metals are dealt with. The independent particle approach to the analysis of two photon angular distributions is discussed and illustrated. A survey of electronic structure investigations includes studies of polycrystalline and single crystal specimens. The relevance of angular correlation measurements in investigations of the Fermi surfaces of metals and alloys is discussed. More recently developed applications to the study of defected and disordered systems are dealt with. A preliminary account of the interpretation of multicomponentmore » lifetime spectra in terms of varying numbers of distinguishable positron states provides the basis for a discussion of studies of positron trapping by defects, voids. and surfaces in ionic and metallic solids, liquids and powders. (auth)« less

Positron studies of condensed matter

A new model of positronium (Ps) formation is proposed. Positronium is assumed to be formed by a reaction between a positron and an electron in the positron spur. Ps formation must compete with electron‐ion recombination and electron or positron reactions with solvent molecules and scavenger impurities. It is also influenced by electron and positron solvation. The model correlates the measured Ps formation probabilities with the spur electron properties determined in radiation chemistry. The predictions of the model are shown to be in good agreement with experimental results for liquids and solids.

Spur reaction model of positronium formation

Positron annihilation spectroscopy (PAS) is a novel method that provides molecular-level information about complex macromolecular structure in a manner different from, but complementary to, conventional physical and chemical methodology. This paper presents a perspective of PAS in polymeric systems covering 12 aspects: historical, spacial, spherical quantum model, anisotropic structure, voids, positronium chemistry, time, positron annihilation lifetime spectroscopy and data analysis, variable monoenergetic slow positron beam techniques and depth profiling, elemental analysis, multidimensional instrumentation advances in PAS, and free volume and free-volume theories.

Perspective of Positron Annihilation Spectroscopy in Polymers

Positron lifetime spectra were measured in mono‐ and polycrystalline light ice, polycrystalline heavy ice, doped light ice, as well as in light and heavy water. All spectra were resolved into three components. At temperatures between −196° and −100°C the lifetimes and relative intensities are virtually constant, being 0.12 nsec and 20%, 0.44 nsec and 28%, 0.68 nsec and 52%, and attributed to annihilation of para‐Ps, free positrons, and ortho‐Ps, respectively. Above −100°C the longest lifetime increases with temperature to 1.1 nsec at 0°C. Its relative intensity is unchanged, while the parameters for the other components show a complex behavior. The spectra for mono‐ and polycrystalline light ice and for polycrystalline heavy ice are identical. For water long lifetime components attributed to ortho‐Ps are 1.86 nsec, 27% for H2O and 2.01 nsec, 22% for D2O. Theoretical explanations are suggested. Fast frozen solutions of HF with concentrations larger than approximately 10−5 mole fraction have a lifetime comp...

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Positron Lifetimes in Pure and Doped Ice and in Water

The parameters of triplet positronium annihilation in 193 organic liquids have been measured. The annihilation quenching cross sections, 〈συ〉A v = (1 / τ2) (M / ρ), is a linear function of the length of the molecule in homologous series of compounds. Partial quenching cross sections, calculated for 27 structural functional groups, are used to calculate annihilation cross sections. The importance of steric effects in the annihilation mechanism is demonstrated in the study of several isomeric systems. Triplet positronium intensities depend upon specific atoms or groups in the molecule, rather than any property of the molecule as a whole. A correlation is also shown between annihilation quenching cross sections and electron polarizabilities as measured from indices of refraction. Several systems which quenched the triplet positronium were examined, e.g., free radicals, quinones, and paramagnetic species.

Charles F. Cook

Papers

Correlation of triplet positronium annihilation parameters with structural and electronic properties of organic liquids.