A mobile positron-lifetime spectrometer for field applications based on β+-γ coincidence

+ -γ coincidence measurement, which has been applied to in-situ examinations of microstructural evolution processes during the fatigue of copper single crystals, is described. Since no sandwich-type geometry is required, it is applicable to all specimen geometries commonly used in materials testing and to the non-destructive testing of engineering parts in service. As a radioactive source ⁷²Se generates the positron-emitting ⁷²As, which provides two positron spectra with maximum energies of 2.5 MeV and 3.3 MeV and a prompt γ quantum of 835 keV. The positrons emitted in the direction towards the specimen pass through a fast plastic scintillator and produce a scintillation signal, thereby losing about 150 keV of their energy. This signal serves as a start signal for the positron-lifetime measurement and is measured in coincidence with the subsequent 511 keV annihilation quantum. After passage through the plastic scintillator the remaining positron energy is still high enough to penetrate deep into the material and to allow for real bulk examinations. The prompt γ quantum may serve as an on-line control of the stability of the electronic system which will be useful under non-constant service conditions in a proposed field application. Received: 8 January 1997/Accepted: 14 March 1997     

Slow positron beam study of corrosion-related defects in pure iron

Corrosion-related defects of pure iron were investigated by measuring Doppler broadening energy spectra (DBES) of positron annihilation and positron annihilation lifetime (PAL). Defect profiles of the S-parameter from DBES as a function of positron incident energy up to 30 keV (i.e. ∼1 μm depth) were analyzed. The DBES data show that S-parameter increases as a function of positron incident energy (mean depth) after corrosion, and the increase in the S-parameter is larger near the surface than in the bulk due to corrosion. Furthermore, information on defect size from PAL data as a function of positron incident energy up to 10 keV (i.e. ∼0.2 μm depth) was analyzed. In the two-state trapping model, the lifetime τ₂ = 500 ps is ascribed to annihilation of positrons in voids with a size of the order of nanometer. τ₁, which decreases with depth from the surface to the bulk, is ascribed to the annihilation of positrons in dislocations and three-dimensional vacancy clusters. The corroded samples show a significant increase in τ₁ and the intensity I₂, and near the surface the corroded iron introduces both voids and large-size three-dimensional vacancy clusters. The size of vacancy clusters decreases with depth.     

Slow positron beam study of nitrogen implanted CZ-Si subjected to rapid thermal processing

In this experiment, nitrogen ions were implanted into CZ-silicon wafer at 100 keV at room temperature with the fluence of 5 × 10¹⁵ N₂⁺/cm², followed by rapid thermal processing (RTP) at different temperatures. The single detector Doppler broadening and coincidence Doppler broadening measurements on slow positron beam were carried out to characterize the defects in the as-implanted silicon and RTP-treated samples. It is found that both nitrogen-vacancy complexes (N-Vsi) and oxygen-vacancy complexes (O-Vsi) produced by nitrogen implantation diffuse back to the sample surface upon annealing. But the N-Vsi and the O-Vsi complete with each other and give a summed effect on positron annihilation characteristics. It is shown that the N-Vsi win out the O-Vsi in as-implanted sample and by RTP at 650 °C, 750 °C, which make the S-parameter increase; O-Vsi plays a dominant role after annealing above 850 °C, which makes the S parameter decrease.     

Polymeric membrane studied using slow positron beam

A radioisotope slow positron beam has been built at the Chung Yuan Christian University in Taiwan for the research and development in membrane science and technology. Doppler broadening energy spectra and positron annihilation lifetime have been measured as a function of positron energy up to 30 keV in a polyamide membrane prepared by the interfacial polymerization between triethylenetetraamine (TETA) and trimesoyl chloride (TMC) on modified porous polyacrylonitrile (PAN) asymmetric membrane. The multilayer structures and free-volume depth profile for this asymmetric membrane system are obtained. Positron annihilation spectroscopy coupled with a slow beam could provide new information about size selectivity of transporting molecules and guidance for molecular designs in polymeric membranes.     

Determination of Protein Levels in Nigerian Grains Using 14 MeV Neutron Activation Analysis

Fast (14 MeV) neutrons have been successfully used in investigating the protein content of different food grains (Soya Beans, Sorghum, Maize and Beans) locally grown and consumed in Nigeria. Protein was estimated via nitrogen using the ¹⁴N(n, 2n)¹³N reaction. Quantification of nitrogen was achieved through a γ-γ coincidence counting of 511 keV positron emissions from the decaying ¹³N. The implication of the use of the emitted annihilation positrons, the interference introduced in the analytical energy spectra from other activated target nuclides present in the sample, as well as possible proton “knock on” reactions anticipated from cellulose in grain matrix were assessed, and their contributions to the 511 keV gamma energy resolved. For comparative purposes, replicates of samples analyzed through Fast Neutron Activation Analysis (FNAA) were investigated using the Kjeldahl method. The samples were carried through the Kjeldahl process of pre-digestion (with appropriate catalysts), digestion and titration. The results obtained through the Kjeldahl process were found to be in good agreement with those obtained using FNAA although slightly lower. Protein content (%) of Nigerian grains analyzed varied from a low 8.75 ± 2.96 for sorghum to 35.93 ± 0.31 for soya beans.     

Performance of a slow positron beam using a hybrid lens design

The University of Hong Kong positron beam employs conventional magnetic field transport to the target, but has a special hybrid lens design around the positron moderator that allows the beam to be focused to millimeter spot sizes at the target. The good focusing capabilities of the beam are made possible by extracting work-function positrons from the moderator in a magnetic field free region using a conventional Soa lens thus minimizing beam canonical angular momentum. An Einzel lens is used to focus the positrons into the magnetic funnel at the end of transportation magnetic field while at the same time bringing up the beam energy to the intermediate value of 7.5 keV. The beam is E × B filtered at this intermediate energy. The final beam energy is obtained by floating the Soa-Einzel system, E × B filter and flight tube, and accelerating the positrons just before the target. External beam steering saddle coils fine tune the position, and the magnetic field around the target chamber is adjusted so as to keep one of the beam foci always on the target. The system is fully computer controlled. Variable energy-Doppler broadened annihilation radiation (VEDBAR) data for a GaN sample are shown which demonstrate the performance of the positron beam system.     

Positron mobility in polyethylene in the 60–400 K temperature range

We have determined the positron mobility (₊) in polyethylene samples (67.2% crystalline, glass transition temperatureT _g=151 K) in the 64–400 K temperature range by Doppler shift measurements. A method based on the simulataneous observation of two lines from¹³³Ba and¹³⁷Cs radioactive sources together with the positron annihilation line, was employed to measure the Doppler shift of the 511 keV line as a function of the electric field applied to the samples. With this method we were able to measure at the same time the drift velocity of positrons and theS parameter. This parameter is very important in the interpretation of the mobility trend in samples where the positron states change with temperature. The positron mobility was corrected for positronium formation. ₊ at 64 K is 31.7±0.8 cm² V^–1 s^–1 then decreases up to 123 K, increases at 148 K and decreases again up to 170 K (₊=26.9±0.8 cm² V^–s^–). This sharp change in mobility is centred around the glass transition temperature of our samples. Then the mobility remains almost constant up to 230 K. From 250 K to 377 K, ₊ increases and reaches the value of 38.4±1.0 cm² V^–1s^–1. The corrected experimental data were well fitted by a simple model taking into account scattering and a thermally activated process (hopping mechanism).     

Orthopositronium annihilation and emission in mesostructured thin silica and silicalite-1 films

Mesoporous silica films and MFI-type pure silica zeolite films were investigated using slow positrons. Detection of the 3γ annihilation fraction was used as a quick test to estimate the emission of orthopositronium (o-Ps) into vacuum. Positronium time-of-flight (TOF) spectroscopy, combined with Monte-Carlo simulation of the detection system was used to determine the energy of o-Ps emitted from the films. Evidence for an efficient o-Ps emission was found in both the mesoporous and silicalite-1. A 3γ fraction in the range of 31-36 % was found in the films with the highest o-Ps yield in each type of porous material, indicating that 40-50 % of the implanted positrons form positronium in the pore systems with very different pore sizes. Time-of-flight measurements showed that the energy of the orthopositronium emitted into vacuum is below 100 meV in the film with 2-3 nm pores at 3 keV positron energy, indicating an efficient slowing down but no complete thermalization in the porous films of 300-400 nm thickness.     

Vacancy defects induced in sintered polished UO2 disks by helium implantation

Vacancy defects have been investigated in sintered polished and annealed uranium oxide disks. Slow positron beam coupled with Doppler broadening spectrometer was used to probe the track region of 1 MeV ³He ions implanted in uranium dioxide (UO₂) disks. The low and high momentum annihilation fractions, S and W, respectively, were measured in the first micrometer near surface region of the disks as a function of positron energy. The S and W values indicate that the 1 MeV He ions induce vacancy defects in the track region of their range. The vacancy defect depth distribution is heterogeneous. The positron trapping at these vacancy defects increases with the depth and with the implantation fluence indicating an increase of the vacancy defect concentration. The nature of the induced vacancy defects does not change with the fluence.     

Study of the effect of annealing on defects in Fe-Mn-Si-Cr-Ni-C alloy by slow positron beam

FeMnSi shape memory alloys (SMAs) have received much attention as one-way SMAs due to their cost-effectiveness. Variable-energy (0-30 keV) positron beam studies have been carried out on a Fe-Mn-Si-Cr-Ni-C alloy with different degrees of deformation. Doppler broadening profiles of the positron annihilation as a function of incident positron energy were shown to be quite sensitive to defects introduced by deformation. The variation of the nature and the concentration of defects are studied as a function of isochronal annealing temperature. These results are correlated with the data measured with the positron annihilation lifetime spectroscopy (PALS). The positron annihilation results are compared to XRD and optical microscopy (OM).     

Status of the pulsed low energy positron beam system (PLEPS) at the Munich Research Reactor FRM-II

The Munich pulsed low energy positron beam system (PLEPS) is now installed at the high intensity positron source (NEPOMUC) at the Munich Research Reactor FRM-II. In order to enhance the performance of the system several improvements have been implemented: two additional collinear detector ports have been installed. Therefore in addition to the normal lifetime measurements it is now possible to simultaneously perform Doppler-broadening, coincident Doppler-broadening and age momentum correlation experiments. An additional chopper was included to periodically suppress pulses and therefore to extend the standard time window of 20 ns for precise measurements of longer lifetimes. First test-experiments have been performed in May and July 2007. With all pulsing components in operation we achieved a count-rate of 1.4 × 10⁴ counts per second. The total time resolution (pulsing and detector) was about 240 ps (FWHM) with a peak to background ratio up to 6 × 10³:1.     

Performance of the Beijing pulsed variable-energy positron beam

In order to study the depth-dependent characteristics of open-volume defects in thin surface layers, the variable-energy positron lifetime spectroscopy (VEPLS) has been enabled by pulsing a continuous positron beam. The buncher is a quarter-wave coaxial resonator and the RF-signal is fed in by a coupling loop with a frequency of 149.89 MHz and the reflection factor of 0.05 measured by a Network Analyzer. Three synchronic signals with their phases and amplitudes adjusted independently are supplied for start signal of the positron lifetime measurement and the power signal by an electronic system. The stop signal is derived from a detector, a BaF₂ scintillator coupled to a photomultiplier-tube (Hamamatsu). The time resolution of 295 ps (FWHM) was achieved for a Kapton film and a Ti sample at positron energies in the range between 1 keV and 30 keV.     

Application of positron annihilation spectroscopy on the ion implantation damaged Fe-Cr alloys

Four different Fe-Cr binary alloys with Cr content 2.5-11 wt% were studied in details using various methods. Transmission electron microscopy (TEM) and X-ray diffraction (XRD) were applied to obtain basic information, required for standard positron annihilation lifetime spectroscopy (PALS) spectra analysis. Additionally, PALS measurements were performed on as-received state as well as on helium implanted specimens. The He implantation was proposed for simulation of radiation damage and obtain high doses even in near surface areas (up to 1 μm). The implantation was based on the SRIM code simulation and next DPA calculations. Final concentration of vacancy type defects were calculated for 250 keV He²⁺ beam and the maximum was determined in 600 μm depth. Such specimens are very suitable for positron beam study of vacancy type defect mobility as a result of thermal treatment, which will be performed simultaneously in the future.     

Hydrogen damage in AISI 304 stainless steel studied by Doppler broadening

Hydrogen damage of AISI 304 stainless steel has been systemically investigated by measuring Doppler broadening of positron annihilation. Defect profiles of the S-parameter, the low-momentum annihilation fraction as a function of positron incident energy up to 30 keV (i.e. ∼1 μm depth) have been analyzed. Experimental results show that hydrogen damage between the surface and the bulk has a significant variation with depth, and strongly depends on the condition of hydrogen-charging, i.e. current density and charging time. It has been suggested that the increase in S-parameter near the surface after hydrogen-charging mainly comes from the formation of voids; however the increase in S-parameter in the bulk after hydrogen-charging mainly comes from the production of structural defects (dislocations). Defect densities induced due to hydrogen-charging in some cases (e.g. dislocation density in the bulk) are estimated based on the simple two-state trapping model.     

Annealing ambient on the evolution of He-induced voids in silicon

The effects of annealing ambient on the He-induced voids in silicon were investigated using the combination of the Doppler broadening spectroscopy using a variable-energy positron beam and cross-section transmission electron microscopy (XTEM). A 〈1 0 0〉-oriented silicon wafer was implanted with He ions at an energy of 15 keV to a dose of 2 × 10¹⁶ cm⁻² at room temperature. Post-implantation, the samples were annealed at a temperature of 1000 °C in the ambient of vacuum, argon, nitrogen, air and oxygen. Positron annihilation spectroscopy (PAS) spectra varied with the annealing ambient. XTEM micrographs demonstrated that the density of He-induced voids could be influenced by the annealing ambient.     

Positron annihilation in large polyatomic molecules. The role of vibrational Feshbach resonances and binding

We analyse the process of rapid positron annihilation in large polyatomic molecules due to positron capture into vibrational Feshbach resonances. Resonant annihilation occurs in molecules which can bind positrons, and we analyse positron binding to alkanes using zero-range potentials. Related questions of spectra of annihilation gamma quanta and molecular fragmentation following annihilation, are discussed briefly.     

Messung der Paarkonversionskoeffizienten von59Co

Internal pair formation propabilities in⁶⁰Ni and⁵⁹Co have been determined by a positron annihilation method. The electrons from the β^?-decay of⁵⁹Fe were measured in triple coincidence with annihilation quanta originating from pairs produced in the deexcitation of the⁵⁹Co nucleus. By this triple coincidence technique it was possible to measure separately the pair formation coefficients Γ for transitions in⁵⁹Co. The observed values Γ_1.29=(3.7±0.4)×10^?5 and Γ_1.10=(0.5±0.1)×10^?5 are in agreement with theoretical calculations forE2-radiation.     

Study of the187W states excited in the (n, γ) reaction

A singles-ray spectrum and a spectrum of summed amplitudes of coinciding pulses (SACP) were measured in the¹⁸⁶W(n, )¹⁸⁷W reaction experiment on the thermal neutron beam. It was for the first time that the data on¹⁸⁷W-transitions were obtained in the excitation energy region from 1500–2500 keV. The neutron binding energy was determined to beB _n=5467.25 (4) keV (statistical error only). In result the level scheme of¹⁸⁷W was developed in the excitation energy interval 1E _f < 3.4=" mev,=" which=" contained=" 105=" levels=" with=" about=" 70=" of=" them=" being=" identified=" for=" the=" first=" time.=" the=" experimental=" values=" for=" summed=" intensities=" of=" two-step=" cascades=" were=" established=" to=" exceed=" those=" predicted=" by=" the=" modern=" statistical=" theory=" (by=" 36±6%).=" this=" is=" explained=" by=" a=" considerable=" contribution=" of=" few-quasiparticle=" components=" to=" wave=" functions=" of=" compound=" and=" intermediate=">     

Annihilation of unthermalized positrons in a silicon single crystal at 77°K

A model is considered for the annihilation of nonrelativistic positrons from quantized states in lattice channels. Annihilation gamma rays of energy over 511 keV have been observed when the positrons from an Na²² source strike a silicon single crystal at 77°K. The experimental results agree well with the proposed model.     

Size dependent electron momentum density distribution in ZnS

In this paper, we present size dependent electron momentum density distribution in ZnS. ZnS nanoparticles of size 3.8 nm and 2.4 nm are synthesized using the chemical route and characterized by X-ray diffraction (XRD). The Compton profile measurements are performed on both the nano-sized as well as bulk ZnS samples employing 59.54 keV gamma-rays from ²⁴¹Am source. The results reveal that the valence electron density in momentum space becomes narrower with reduction of particle size. To evaluate the charge transfer on compound formation, the ionic model based calculations for a number of configurations of Zn^+xS^−x (0.0≤x≤2) are also performed utilizing free atom Compton profiles. These results suggest different amounts of charge transfer in these materials varying from 1.2 to 2.0 electron from Zn to S atom.