Positron annihilation spectroscopy method

K. Saarinen, P. Hautojdrvi, and C. Corbel, Positron Annihilation Spectroscopy of Defects in Semiconductors R. Jones and P. R. Briddon, The Ab Initio Cluster Method and the Dynamics of Defects in Semiconductors... 

Abstract This chapter demonstrates the applicability of positrons in nuclear chemistry and material sciences. From the very basics to highly developed spectroscopic methods, a brief outline of positron annihilation spectroscopies is given. The possibilities of these methods are emphasized, and the characteristic applications are outlined for every one of them. 

As positron annihilation spectroscopies are not conventional methods in studying materials, this chapter might need a more basic introduction than others. Consequently, the very basics of positron annihilation spectroscopies, along with most variations of spectroscopies applying positrons as probes for material properties, are explained below. 

The study of defects in metals and semiconductors is still the largest subsection of the applications of positron annihilation spectroscopies demonstrating the use of these methods in metal and semiconductor physics. Both bulk measurements with Na sources and surface studies with low-energy beams are frequent. 

One of the new techniques to scan membranes and determine pore size distributions is positron, annihilation spectroscopy (PAS). With this method also the free spaces in nanofiltration membranes can be determined. For instance in a study by Boussu et al. [9] it was found that some much-studied NF membranes (like Desal-5 DL, NTR7450) have two sizes of spaces, one size about 0.12-0.15 nm and the other between 3nm and 4nm. It could be speculated that diffusive transport would happen through the smaller spaces (the size of a water molecule), depending on the hydrophilicity properties of the membrane, and convective transport through the larger spaces, depending on size and charge conditions. 

Apart from the theoretical approaches, electronic energy spectra of carbides and nitrides have been studied using a variety of experimental techniques X-ray emission and photoelectron spectrosopy, optical and Auger spectroscopy, electron energy loss and positron annihilation spectroscopy, etc. However, interpretation of the results obtained requires, as a rule, use of the computational methods of the band theory of solids and quantum chemistry. Moreover, the data provided by theoretical methods are important by themselves, because they give much more detailed information on the electron states and chemical bonding than any of the experimental methods. They also allow us to model theoretically... 

Utilising new non-destructive spectroscopic methods such as positron annihilation spectroscopy and Mossbauer spectroscopy to test materials used in the nuclear industry and... 

One of the main tasks of nuclear-reactor safety research is assessing the integrity of the reactor pressure vessel (RPV). The properties of RPV steels and the influences of thermal and neutron treatments on them are routinely investigated by macroscopic methods such as Charpy V-notch and tensile tests. It turns out that the embrittlement of steel is a very complex process that depends on many factors (thermal and radiation treatment, chemical compositions, conditions during preparation, ageing, etc.). A number of semi-empirical laws based on macroscopic data have been established, but unfortunately these laws are never completely consistent with all data and do not yield the required accuracy. Therefore, many additional test methods are needed to unravel the complex microscopic mechanisms responsible for RPV steel embrittlement. Our study is based on experimental data obtained when positron annihilation spectroscopy (PAS) and Mdssbauer spectroscopy (MS) were applied to different RPV steel specimens, which are supported by results from transmission electron microscopy (TEM) and appropriate computer simulations. 

In particular, the most powerful method for studing lattice defects, due to the high sensitivity of positrons to open volume defects such as vacancies, vacancy clusters, voids, dislocations, grain boundaries, etc., is positron annihilation spectroscopy (PAS). A diagram illustrating the applicability of PAS and other techniques as a function of defect size and density versus depth in material is shown in Figure 4.25. Thus, PAS represents a non-local experimental technique that is sensitive to microstructural defects at the atomic scale. A well-established theory of positron annihilation phenomena is currently available. Especially for metallic materials, it is possible to perform ab initio calculations of positron parameters for various defects and atomic arrangements [72,73]. 

In this work positron annihilation lifetime spectroscopy (PALS) was used to investigate structural diversity inside zeolite precursor matrix caused by the presence of alkali cations Na, K, Rb and Cs. PALS is an established and well-proven method for structural investigations of various materials, extensively used for metals and alloys, semiconductors and porous materials [3, 4]. In the investigations of zeolites PALS has been mostly used for their void structure and size study [5, 6, 7, 8], also in correlation to... 

Positron annihilation lifetime spectroscopy (PALS) provides a method for studying changes in free volume and defect concentration in polymers and other materials [1,2]. A positron can either annihilate as a free positron with an electron in the material or capture an electron from the material and form a bound state, called a positronium atom. Pnra-positroniums (p-Ps), in which the spins of the positron and the electron are anti-parallel, have a mean lifetime of 0.125 ns. Ortho-positroniums (o-Ps), in which the spins of the two particles are parallel, have a mean lifteime of 142 ns in vacuum. In polymers find other condensed matter, the lifetime of o-Ps is shortened to 1-5 ns because of pick-off of the positron by electrons of antiparallel spin in the surrounding medium. 

A new spectroscopic method for the characterization of surface vacancy clusters is a combination of positron lifetime spectroscopy, which determines the size of vacancy clusters, and coincidence Doppler broadening of annihilation radiation, which gives information on where vacancy clusters are located [5, 6]. If these clusters are located on the surface of gold nanoparticles, namely the interface between the particle and host matrix, the surroundings of the clusters should include both particle atoms and the matrix atoms. Doppler broadening of annihilation radiation (DBAR) with two-detector coincidence should be able to reveal these atomic constituents, and therefore elucidate the location of vacancy clusters. 

The objectives of this research are basically two firstly, to analyze the use of positron annihilation lifetime spectroscopy to the study of carbon materials with high surface area and, secondly, to get a correlation between the parameters observed in PALS experiments and the results obtained in the characterization of porous materials by well-known methods like gas adsorption and Small Angle X-Ray Scattering (SAXS). 

In crystals, impurities can take simple configurations. But depending on their concentration, diffusion coefficient, or chemical properties and also on the presence of different kind of impurities or of lattice defects, more complex situations can be found. Apart from indirect information like electrical measurements or X-ray diffraction, methods such as optical spectroscopy under uniaxial stress, electron spin resonance, channelling, positron annihilation or Extended X-ray Absorption Fine Structure (EXAFS) can provide more detailed results on the location and atomic structure of impurities and defects in crystals. Here, we describe the simplest atomic structures more complicated structures are discussed in other chapters. To explain the locations of the impurities and defects whose optical properties are discussed in this book, an account of the most common crystal structures mentioned is given in Appendix B. 

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