Interaction of hydrogen and deuterium with intrinsic atomic defects in high-purity electron-irradiated nickel

Abstract

High-purity nickel was irradiated with 2 MeV electrons at temperatures below 80 K to a dose of 1 × 10²³ e^?/m² in the as-prepared state and after charging with H or D. By means of magnetic after-effect measurements relaxations of anisotropic radiation-induced defects and of defect-hydrogen complexes were investigated in the temperature range between 4.2 and 500 K. The isochronal annealing behaviour of these relaxations and the isochronal recovery of the residual resistivity was measured simultaneously on the same specimens. At temperatures below the hydrogen mobility (< 160 K) in charged irradiated specimens relaxation maxima are observed at 45, 100, 115 and 140 K which show no isotope shift for H and D charging. The maxima below 160 K are explained by defect-hydrogen complexes, where radiation-induced defects reorient around immobile hydrogen atoms. Above 160 K, where hydrogen atoms get mobile, in charged irradiated specimens a broad relaxation maximum appears at 170 K which shows an inverse isotope shift for H and D charging. This 170 K maximum anneals in Stage III. A hydrogen diffusion maximum observed in charged specimens at 215 K prior to irradiation is missing after electron irradiation. The 170 K relaxation is explained by defect-hydrogen complexes, where hydrogen atoms reorient around immobile radiation-induced defects while the long-range hydrogen diffusion is suppressed by these defects. In such relaxation measurements hydrogen and deuterium atoms are used as a “probe” to investigate radiation-induced defects.     

Effect of proton irradiation on the physical properties of PC/PBT blends

Samples from polycarbonate/poly (butylene terephthalate) (PC/PBT) blends film have been irradiated using different fluences (1?×?10¹⁵– 5?×?10¹⁷ H⁺/cm²) of 1?MeV protons at the University of Surrey Ion Beam Center, UK. The structural modi?cations in the proton irradiated samples have been studied as a function of fluence using different characterization techniques such as X-ray diffraction and UV spectroscopy. The results indicate that the proton irradiation reduces the optical energy gap that could be attributed to the increase in structural disorder of the irradiated samples due to crosslinking. Furthermore, the color intensity ΔE, which is the color difference between the non-irradiated sample and those irradiated with different proton fluences, increased with increasing the proton fluence up to 5?×?10¹⁷ H^+/cm², convoyed by an increase in the red and yellow color components. In addition, the resultant effect of proton irradiation on the thermal properties of the PC/PBT samples has been investigated using thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). It is found that the PC/PBT decomposes in one weight loss stage. Also, the variation of transition temperatures with proton fluence has been determined using DSC. The PC/PBT thermograms were characterized by the appearance of two endothermic peaks due to the glass transition and melting temperatures. The melting temperature of the polymer, T_m, was investigated to probe the crystalline domains of the polymer, since the proton irradiation destroys the crystalline structure so reducing the melting temperature.     

Electron beam effects on oxygen exposed aluminum surfaces

The damaging effects of electron beams during the acquisition of electron spectra have long been an obstacle in surface analysis. In order to understand the physico-chemical processes which take place under electron irradiation in an AlO system, we have carried out an experiment in which artifices, such as heating, charging, and gas contamination, were absent. We have observed with Auger Electron Spectra increases of the oxidation extent and the oxygen concentration on an oxygen exposed (111) textured polycrystalline surface under electron irradiation (5 keV, 9 × 10^?5 A/cm²). These increases were not observed on a clean surface, and were very feeble on a (100) single crystal surface. The increase of oxygen concentration was independent of residual gas pressure (3 × 10^?9 to 6 × 10^?10 Torr) and its composition; and therefore cannot be explained by gas contamination during the experimental period (about 70 min). We attribute the increase of oxidation degree to the transition of chemisorbed oxygen atoms into oxide through direct momentum transfer from the incident electrons. We suggest that the increase of oxygen within the irradiated area is due to the surface diffusion of chemisorbed oxygen atoms from outside the irradiated area. These oxygen atoms are excited by the electrons scattered from the vacuum chamber walls and gain energy through Franck-Condon type mechanism. The absence of chemisorbed oxygen atoms on (100) surface explains the near absence of these increases on this surface.     

Subthreshold sputtering at high temperatures

The sputtering of tungsten from a target at a temperature of 1470 K during irradiation by 5-eV deuterium ions in a steady-state dense plasma is discovered. The literature values of the threshold for the sputtering of tungsten by deuterium ions are 160–200 eV. The tungsten sputtering coefficient measured by the loss of weight is found to be 1.5×10^?4 atom/ion at a deuterium ion energy of 5 eV. Previously, such a sputtering coefficient was usually observed at energies of 250 eV. The sputtering is accompanied by a change in the target surface relief, i.e., by the etching of the grain boundaries and the formation of a wavy structure on the tungsten surface. The subthreshold sputtering at a high temperature is explained by the possible sputtering of adsorbed tungsten atoms that are released from the traps around the interstitial atoms and come to the target surface from the space between the grains. The wavy structure on the surface results from the merging of adsorbed atoms into ordered clusters.     

Hydrogen isotope accumulation in a vanadium alloy under different irradiations and the long-range interaction effect

Hydrogen and deuterium accumulation after irradiation of a vanadium alloy V-3.5 Ga with pulsed and steady-state plasma and hydrogen ions with a dose of 1.0 × 10¹⁹ cm^?2 has been studied. Hydrogen and deuterium saturation of surface layers 15–40 nm thick has been detected to occur both on the sides of irradiated and nonirradiated targets. Possible mechanisms of the observed effects are discussed.     

Transmutation doping of GaAs by thermal neutrons

The electrical properties of GaAs have been modified by transmutation of about 1 × 10¹⁸ As atoms per cm³ to Se and 0.7 × 10¹⁸ Ga atoms per cm³ to Ge in a flux of thermal neutrons, followed by annealing at temperatures from 625 to 900°C. Enhancement of carrier concentration was not observed in n⁺ samples, although p and n^? material showed changes in carrier concentration of the expected magnitude.     

Study of plastic deformation and proton irradiation influence on phase transitions in C18N9T stainless steel

Transmission and post-nuclear-reaction emission Mössbauer spectroscopy was used for investigation of radiation effects and plastic deformation influence on C18N9T steel. The rolled foil was annealed in 10^?6 Torr vacuum at 870 K during 2 hours and was irradiated by 30 MeV protons at current density of 0.8μ A up to doses of 5×10¹⁷ cm^?2 on the isochronous cyclotron at the liquid nitrogen cooling of the target. The Mössbauer spectra obtained before and after the sample irradiation in transmission geometry are identical. The emission spectrum is analogous to the spectrum of the plastically deformed sample. It is concluded that during irradiation in the steel the processes take place which are similar to those at plastic deformation and connected with redistribution of the alloy component atoms.     

Effect of MeV electron irradiation on the free volume of polyimide

The free volume of the microvoids in the polyimide samples, irradiated with 6 MeV electrons, was measured by the positron annihilation technique. The free volume initially decreased the virgin value from ～13.70 to ～10.98 Å³ and then increased to ～18.11 Å³ with increasing the electron fluence, over the range of 5?×?10¹⁴ – 5?×?10¹⁵ e/cm². The evolution of gaseous species from the polyimide during electron irradiation was confirmed by the residual gas analysis technique. The polyimide samples irradiated with 6 MeV electrons in AgNO₃ solution were studied with the Rutherford back scattering technique. The diffusion of silver in these polyimide samples was observed for fluences >2?×?10¹⁵ e/cm², at which microvoids of size ≥3 Å are produced. Silver atoms did not diffuse in the polyimide samples, which were first irradiated with electrons and then immersed in AgNO₃ solution. These results indicate that during electron irradiation, the microvoids with size ≥3 Å were retained in the surface region through which silver atoms of size ～2.88 Å could diffuse into the polyimide. The average depth of diffusion of silver atoms in the polyimide was ～2.5 μm.     

Coverage of foreign atoms on surfaces as a function of adsorption,sputtering, and diffusion rates

During sputtering of a surface the coverage of foreign atoms may be changed by diffusion from the bulk to the surface and by adsorption from the gas phase. Assuming sufficiently high negative surface segregation enthalpy i.e. high ratios of surface to bulk concentration in equilibrium, simple expressions of the coverage time function for finite and semi-infinite samples are derived. The equations were applied to experimental results of oxygen coverage on a niobium surface where the three processes mentioned above were active. From the comparison with these results the diffusion coefficients of O in Nb D = 2 × 10^?13 m²/s at 520°C and D = 9 × 10^?13 m²/s at 600°C were evaluated.     

Influence of the defect state of samples on the luminescence spectra of CdS single crystals irradiated by electrons

The photoluminescence spectra of CdS single crystals irradiated by electrons (E = 1.2 MeV, Φ = 2×10¹⁷ cm^?2) are investigated in the visible and near-infrared regions of electromagnetic radiation. Some samples of the CdS single crystals are preliminarily irradiated by neutrons (E = 2 MeV, Φ = 2 × 10¹⁸ cm^?2) with the aim of increasing the concentration of initial structural defects. From analyzing the peak intensities of photoluminescence in the irradiated single crystals at the wavelengths λ_m = 0.720, 1.030, and 0.605 μm, it is concluded that the CdS samples with a low concentration of structural defects in the initial state possess the highest resistance to electron radiation. It is assumed that the observed transformation of the photoluminescence spectra of the imperfect CdS single crystals subjected to electron irradiation is determined by either the mechanisms of subthreshold defect formation or the transformation of the defect complexes in elastic and electric fields near the large structural damages of the crystal lattice.     

Studies of some physical properties of PrFe0.7Ni0.3O3 thin films after 200 MeV Ag15+ irradiation

PrFe_0.7Ni_0.3O₃ thin films (thickness ~ 200 nm) were prepared by pulsed laser ablation technique on LaAlO₃ substrate. These films were irradiated with 200?MeV Ag¹⁵⁺ ions at various fluencies, ranging from 1 × 10¹¹ to 1 × 10¹² ions/cm². These irradiated thin films were characterized by using X-ray diffraction, dc conductivity, dc magnetization and atomic force microscopy. These films exhibit orthorhombic structure and retain it even after irradiations. The crystallite size (110–137?nm), micro strain (1.48 × 10^?2–1.75 × 10^?2 line^?2?m^?4) and dislocation density (79.7 × 10¹⁴–53.2 × 10¹⁴ line/m²) vary with ion fluencies. An enhancement in resistivity at certain fluence and then a decrease in its value (0.22175–0.21813?Ω?cm) are seen. A drastic change in observed magnetism after ion irradiation is seen. With ion irradiation, an increase in surface roughness, due to the formation of hillocks and other factors, is observed. Destruction of magnetic domains after irradiation can also be visualized with magnetic force microscopy and is in close agreement with magnetization data. The impact on various physical properties in these thin films after irradiation indicates a distortion in the lattice structure and consequently on single-particle band width caused by stress-induced defects.     

Microstructural evolution and changes in mechanical property of irradiated Fe–0.6Cu alloy under uniaxial tension stress in reactor

Structural materials for commercial reactor are usually used under conditions of stress. However, the evaluation of the microstructural evolution and the changes in the mechanical property induced by the neutron irradiation in structural materials does not typically consider the effect of stress since it is difficult to carry out neutron irradiation testing under conditions of stress. In this study, a model alloy (Fe–0.6Cu) of reactor pressure vessels was irradiated by neutrons at 573?K with a dose of about 3.2?×?10²¹?neutrons/m² (E?>?0.1?MeV), corresponding to 5.2?×?10^?4?dpa (displacement per atom), with and without tension stress. The tension stress caused elastic deformation in the specimens. The size of microvoids in the irradiated sample with tension stress was larger than that in the sample without tension stress. However, the effects of stress on the formation of Cu precipitates and the changes in the mechanical property were not clear.     

Mixing of Au in Si induced by secondary and high-order recoil implantation

The mixing of Au in Si induced by secondary and high-order recoil implantation was investigated using 350 keV Ar⁺ and 350 keV Kr⁺ ions to fluences from 1?×?10¹⁶ to 3?×?10¹⁶ ions/cm² at room temperature. The thickness of the Au layer evaporated on Si substrate was ～2400 Å.The ranges of the Ar and Kr ions were chosen to be lower than the thickness of the Au layer in order to avoid the ballistic mixing produced by the primary knock-on atoms. Rutherford backscattering spectrometry (RBS) experiments were carried out to study the effects induced by Ar and Kr irradiation at the interface of Au–Si system. We observed that in the case of the irradiation with Ar⁺ ions, a broadening of the Au–Si interface occurred only at the fluence of 3?×?10¹⁶ Ar⁺/cm² and it is attributed to the surface roughening induced by ion bombardment. In contrast, the RBS analysis of a sample irradiated with 2?×?10¹⁶ Kr⁺/cm² clearly showed, in addition to the broadening effect, the formation of a mixed zone of Au and Si atoms at the interface. The mixing of Au in Si atoms can be explained by the secondary and high-order recoil implantation followed by subsequent collision cascades.     

50 MeV Li3+ ion irradiation effect on structural, electrical, and dielectric properties of PVA-based nanocomposite polymer electrolytes

Nanocomposite polymer electrolyte thin films of polyvinyl alcohol (PVA)-orthophosphoric acid (H₃PO₄)-Al₂O₃ have been prepared by solution cast technique. Films are irradiated with 50 MeV Li³⁺ ions having four different fluences viz. 5?×?10¹⁰, 1?×?10¹¹, 5?×?10¹¹, and 1?×?10¹² ions/cm². The effect of irradiation on polymeric samples has been studied and characterized. X-ray diffraction spectra reveal that percent degree of crystallinity of samples decrease with ion fluences. Glass transition and melting temperatures have been also decreased as observed in differential scanning calorimetry. A possible complexation/interaction has been shown by Fourier transform infrared spectroscopy. Temperature-dependent ionic conductivity shows an Arrhenius behavior before and after glass transition temperature. It is observed that ionic conductivity increases with ion fluences and after a critical fluence, it starts to decrease. Maximum ionic conductivity of ～2.3?×?10^?5 S/cm owing to minimum activation energy of ～0.012 eV has been observed for irradiated electrolyte sample at fluence of 5?×?10¹¹ ions/cm². The dielectric constant and dielectric loss also increase with ion fluences while they decrease with frequency. Transference number of ions shows that the samples are of purely ionic in nature before and after ion irradiation.     

Deuterium accumulation in tungsten under low-energy high-flux plasma exposure

The accumulation of deuterium implanted in tungsten is simulated within the framework of kinetic diffusion theory. The influence of the tungsten microstructure (dislocation density and impurity concentration) on the process of deuterium capture and accumulation is considered. It is established that, under the chosen irradiation conditions, deuterium accumulation in the near-surface region is determined by capture at defects formed during implantation. The deuterium concentration gradient, together with the material microstructure, determines its accumulation in tungsten. Variation in the dislocation density and impurity concentration does not affect the simulation results, which is, first, related to the fact that the model used does not contain alternative mechanisms for the formation and growth of vacancy clusters under the subthreshold irradiation mode. The simulation results are compared with experimental data, and ways of improving the model are discussed in order to explain the deuterium-saturation effect for high fluences (more than 10²³ m^?2).     

Swift heavy ion provoked structural, optical and electrical properties in SnO2 thin films

SnO₂ thin films grown on glass substrates at 300 ^°C by reactive thermal evaporation and annealed at 600 ^°C were irradiated by 120 MeV Ag⁹⁺ ions. Though irradiation is known to induce lattice disorder and suppression of crystallinity, we observe grain growth at a certain fluence of irradiation. X-ray diffraction (XRD) revealed the crystalline nature of the films. The particle size estimated by Scherrer’s formula for the irradiated films was in the range 10–25 nm. The crystallite size increases with increase in fluence up to 1×10¹² ions?cm^?2, whereas after that the size starts decreasing. Atomic force microscope (AFM) results showed the surface modification of nanostructures for films irradiated with fluences of 1×10¹¹ ions?cm^?2 to 1×10¹³ ions?cm^?2. The UV–visible spectrum showed the band gap of the irradiated films in the range of 3.56 eV–3.95 eV. The resistivity decreases with fluence up to 5×10¹² ions?cm^?2 and starts increasing after that. Rutherford Backscattering (RBS) reveals the composition of the films and sputtering of ions due to irradiation at higher fluence.     

Migration behaviour of vacancies and damage structure recovery in a Fe-based Fe-Cr-Mn-Cu-Mo multi-component alloy

ABSTRACT

A Fe-based multi-component alloy, 60Fe-12Cr-10Mn-15Cu-3Mo, which presents higher yield stress than typical stainless steels (such as 304, 316, and 340), was used to investigate the thermal stability of irradiation-induced defects. Neutron irradiation was carried out at approximately 323 and 643?K using up to 1.3 × 10^?3 and 4.5 × 10^?4 dpa (displacements per atom), respectively. While no defects were accumulated at the high temperature of 643?K, single vacancies were formed after irradiation at the low temperature of 323?K to 1.3 × 10^?3 dpa, and the vacancies became mobile at 423?K. As a result, vacancy clusters were formed. However, as the annealing temperature increased the size of vacancy clusters decreased. Coincidence Doppler broadening measurements indicated that Cu precipitates were the sites of vacancy cluster formation, and the recovery of vacancy clusters became prominent while annealing the irradiated sample at temperatures higher than 423?K. Recovery of vacancy clusters at 573?K, which was not a high temperature, was also observed even in the sample that was irradiated using 2.5?MeV Fe ions at room temperature to 0.6 dpa at damage peak.     

Superior tolerance of Ag/Ni multilayers against Kr ion irradiation: an in situ study

Monolithic Ag and Ni films and Ag/Ni multilayers with individual layer thickness of 5 and 50?nm were subjected to in situ Kr ion irradiation at room temperature to 1 displacement-per-atom (a fluence of 2?×?10¹⁴?ions/cm²). Monolithic Ag has high density of small loops (4?nm in diameter), whereas Ni has fewer but much greater loops (exceeding 20?nm). In comparison, dislocation loops, ～4?nm in diameter, were the major defects in the irradiated Ag/Ni 50?nm film, while the loops were barely observed in the Ag/Ni 5?nm film. At 0.2?dpa (0.4?×?10¹⁴?ions/cm), defect density in both monolithic Ag and Ni saturated at 1.6 and 0.2?×?10²³/m³, compared with 0.8?×?10²³/m³ in Ag/Ni 50?nm multilayer at a saturation fluence of ～1?dpa (2?×?10¹⁴?ions/cm²). Direct observations of frequent loop absorption by layer interfaces suggest that these interfaces are efficient defect sinks. Ag/Ni 5?nm multilayer showed a superior morphological stability against radiation compared to Ag/Ni 50?nm film.     

Study of the Elution Profile of the 99mTc Gel Generator

The generator with gel matrix is considered a perspective type for obtaining ^99mTc. The elution yield of a generator and the course of the elution profile A_Vn = f(V_n) are affected by the properties and conditions of preparation of zirconium molybdate (generator matrix). Furthermore, it is influended by neutron flux density as well as irradiation time and temperature of cooling water during the irradiation. Zirconium molybdate, Mo: Zr = 1.72, in the form of a monodispersion (mean particle size x = 0.175 mm), was irradiated under the neutron flux density ?_n = (0.7 … 2.2) × 10¹³ cm^?2 s^?1. The elution profile and the elution yield of ^99mTc were examined in dependence on the temperature of drying the Zr–Mo matrix (40–100 °C). The kinetics of the passage of ^99mTc into the solution, in dependence on the temperature of drying the hydrogel, was investigated. Some predetermined substitutional functions were tested and the mechanism of the ^99mTc passage into solution was explained.     

Defect sites in thin films of germanium dioxide irradiated with silicon ions

Optical transmission spectra of GeO₂ films irradiated with silicon ions and subjected to postimplantation annealing in the regime of silicon nanocrystal formation are analyzed. It is shown that point defects form in the films after irradiation with doses D ～ 10²⁰ m^?2: germanium electron centers, neutral oxygen vacancies, and Ge²⁺ centers, which have been annealed at a temperature of 1000°C for an hour. At D ≥ 1 × 10²¹ m^?2, more complex defects arise in the films, which are only partially annealed under the same conditions.