Effect of tin on the irradiation growth of polycrystalline zirconium

Measurements of irradiation growth of polycrystalline Zr-1.5% Sn and Zr-0.1% Sn alloys at 353 K and 553 K have been made following fast neutron irradiation with fluences up to 3.1 × 10²⁵ n/m². At 353 K, growth of Zr-1.5% Sn virtually saturated at a strain of 4.5 × 10⁻⁴ after a fluence of ˜10²⁴ n/m². At this temperature, Zr-0.1% Sn continued to grów until ˜ 2 × 10²⁵ n/m², when the strain levelled off at ˜ 1.2×10⁻³. At 553 K, Zr-1.5% Sn initially grew about twice as fast as the 0.1% Sn alloy, but both eventually reached the same steady state rate of ˜ 2.4 × 10⁻²⁹ m²/n. Comparison of the data for the 1.5% Sn material with those for Zircaloy-2 from earlier work reveals that at 353 K, growth is suppressed by the presence of Sn atoms, which may serve as vacancy traps. However, at 553 K, minor additions and impurities in Zircaloy-2 (such as Fe, Ni, Cr and O) play an important role and cannot be neglected. The growth behaviour of Zr-0.1% Sn is similar to that of pure polycrystalline zirconium, especially at 353 K, indicating that the addition of Sn at this concentration does not strongly influence the growth of zirconium.     

Low temperature fast-neutron and gamma irradiation of glass fiber-epoxy composite. Part 2: Structure and chemistry

Structure and chemistry of S2-glass fiber-epoxy composite to fast-neutron and gamma irradiation at 4.2 K have been studied. Fast-neutron fluence ranged from 0.9 × 10²² to 1 × 10²³ n/m². At the neutron fluence of 3.1 × 10²² n/m², ordering of the amorphous S2-glass structure intervened. Ordering was followed by partial crystallization at the neutron fluence of 1 × 10²³ n/m². Although the epoxy matrix retained its amorphous structure, reactor irradiation induced crosslink formation and hydrogen evolution. These processes became significant at neutron fluences equal to or higher than 1.8 × 10²² n/m². No evidence has been found for hydrogen bubble or void nucleation at the glass-epoxy interface at the neutron fluence of 3.1 × 10²² n/m². Futhermore, sharp compositional changes measured at the glass-epoxy interface preclude an extended irradiation-induced atom mixing at this neutron fluence.     

Investigation of in-reactor creep and irradiation growth of zirconium-2.5 wt% niobium channel tubes

We summarize the diametral creep results obtained in the MR reactor of the Kurchatov Institute of Atomic Energy on zirconium-2.5 wt% niobium pressure tubes of the type used in RBMK-1000 power reactors. The experiments that lasted up to 30 000 h cover a temperature range of 270 to 350°C, neutron fluxes between 0.6 and 4.0 ×10¹³ n/cm² · s (E > 1 MeV) and stresses of up to 16 kgf/mm². Diametral strains of up to 4.8% have been measured. In-reactor creep results have been analyzed in terms of thermal and irradiation creep components assuming them to be additive. The thermal creep rate is given by a relationship of the type ε_th = A₁ exp [(A₂ + A _3σt) T] and the irradiation component by ε_rad = A_4σtø(T − A₅), where T = temperature, σ_t = hoop stress, ø = neutron flux and a₁ to A₅ are constants. Irradiation growth experiments carried out at 280° C on specimens machined from pressure tubes showed a non-linear dependence of growth strain on neutron fluence up to neutron fluences of 5 × 10²⁰ n/cm². The significance of these results to the elongation of RBMK reactor pressure tubes is discussed.     

Heavy ion irradiation effects in the rare-earth sesquioxide Dy2O3

Polycrystalline pellets of the rare-earth sesquioxide Dy₂O₃ with cubic C-type rare-earth structure were irradiated with 300 keV Kr²⁺ ions at fluences up to 5 × 10²⁰ Kr/m² at cryogenic temperature. Irradiation-induced microstructural evolution is characterized using grazing incidence X-ray diffraction (GIXRD) and transmission electron microscopy (TEM). In previous work, we found a phase transformation from a cubic, C-type to a monoclinic, B-type (C2/m) rare-earth structure in Dy₂O₃ during Kr²⁺ ion irradiation at a fluence of less than 1 × 10²⁰ Kr/m². In this study, we find that the crystal structure of the top and middle regions of the implanted layer transform to a hexagonal, H-type (P6₃/mmc) rare-earth structure when the irradiation fluence is increased to 5 × 10²⁰ Kr/m²; the bottom of the implanted layer, on the other hand, remains in a monoclinic phase. The irradiation dose dependence of the C-to-B-to-H phase transformation observed in Dy₂O₃ appears to be closely related to the temperature and pressure dependence of the phases observed in the phase diagram. These transformations are also accompanied by a decrease in molecular volume (or density increase) of approximately 9% and 8%, respectively, which is an unusual radiation damage behavior.     

Helium retention of vanadium alloy after energetic helium ion irradiation

Helium irradiation experiments of V–4Ti alloy were conducted in an ECR ion irradiation apparatus by using helium ions with energy of 5 keV. The ion fluence was in the range from 1 × 10¹⁷ He/cm² to 8 × 10¹⁷ He/cm². After the helium ion irradiation, the helium retention was examined by using a technique of thermal desorption spectroscopy (TDS). After the irradiation, the blisters with a size of about 0.1 μm were observed at the surface, and the blister density increased with the ion fluence. Two desorption peaks were observed at approximately 500 and 1200 K in the thermal desorption spectrum. When the ion fluence was low, the retained helium desorbed mainly at the higher temperature regime. As increase of the ion fluence, the desorption at the lower temperature peak increased and the retained amount of helium saturated. The saturated amount was approximately 2.5 × 10¹⁷ He/cm². This value was comparable with those of the other plasma facing materials such as graphite.     

An assessment of the influence of microstructure and test conditions on the irradiation growth phenomenon in zirconium alloys

Experiments have been carried out to study the irradiation growth phenomenon in zirconium and its alloys. Polycrystalline zirconium, annealed and cold-worked Zircaloy-2, and annealed Zr-2.5%Nb have been irradiated at 353 and 553 K up to neutron doses of 5 × 10²⁵ n/m². Dimensional changes occurring in-reactor and during post-irradiation heat treatment were measured. The results are interpreted in terms of the present understanding of the physical processes involved in the irradiation growth phenomenon.     

Neutron-irradiation effect in ceramics evaluated from macroscopic property changes in as-irradiated and annealed specimens

Macroscopic length (linear swelling) and thermal diffusivity changes were measured for heavily neutron-irradiated -Al₂O₃, AlN, β-Si₃N₄ and β-SiC that were irradiated under the same capsule to compare the difference between these materials. And in addition, several capsules were irradiated under different temperatures (646–1039 K) and to different neutron doses (0.4–8.0 × 10²⁶ n/m²) in the Japanese experimental fast reactor JOYO. The swelling and the thermal diffusivity of as-irradiated specimens showed some dependence on the neutron-irradiation dose and the irradiation temperature, and that indicates stability under neutron-irradiation environments. Alpha-Al₂O₃ and AlN showed relatively large swelling and degradation of thermal diffusivity than β-Si₃N₄ and β-SiC. This difference is related to the crystal structure of each material. The dependence of swelling on irradiation dose, that is, -Al₂O₃ showed linear inclination but β-Si₃N₄ and β-SiC showed saturation, supports the model of defect structures. In addition, annealing behaviors of swelling and thermal diffusivity were compared to analyze the behavior of defects at higher temperature.     

Study of 160 MeV Ni ion irradiation effects on electrodeposited polypyrrole films

Conducting polymer polypyrrole thin films doped with LiCF₃SO₃, [CH₃(CH₂)₃]₄NBF₄ and [CH₃(CH₂)₃]₄NPF₆ have been electrodeposited potentiodynamically on ITO coated glass substrate. The polymer films are irradiated with 160 MeV Ni¹²⁺ ions at three different fluences of 5 × 10¹⁰, 5 × 10¹¹ and 3 × 10¹² ions cm⁻². An increase in dc conductivity of polypyrrole films from 100 S/cm to 170 S/cm after irradiation with highest fluence is observed in four-probe measurement. X-ray diffractogram shows increase in the crystallinity of the polypyrrole films upon SHI irradiation, which goes on increasing with the increase in fluence. Absorption intensity increase in the higher wavelength region is observed in the UV–Vis spectra. The SEM studies show that the cauliflower like flaky microstructure of the surface of polypyrrole films turns globular upon SHI irradiation at fluence 5 × 10¹¹ ions cm⁻² and becomes smooth and dense at the highest fluence used. The cyclic voltammetry studies exhibit that the redox properties of the polypyrrole films do not change much on SHI irradiation.     

Effects of 160 MeV Ni ion irradiation on polypyrrole conducting polymer electrode materials for all polymer redox supercapacitor

Electronically conducting polymers are suitable electrode materials for high performance supercapacitors, for their high specific capacitance and high dc conductivity in the charged state. Supercapacitors and batteries are energy storage and conversion systems which satisfies the requirements of high specific power and energy in a complementary way. Ion beam {energy > 1 MeV} irradiation on the polymer is a novel technique to enhance or alter the properties like conductivity, density, chain length and solubility.

Conducting polymer polypyrrole thin films doped with LiClO₄ are synthesized electrochemically on ITO coated glass substrate and are irradiated with 160 MeV Ni¹²⁺ ions at different fluence 5 × 10¹⁰, 5 × 10¹¹ and 3 × 10¹² ions cm⁻². Dc conductivity measurement of the irradiated films showed 50–60% increase in conductivity which is may be due to increase of carrier concentration in the polymer film as observed in UV–Vis spectroscopy and other effects like cross-linking of polymer chain, bond breaking and creation of defects sites. X-ray diffractogram study shows that the degree of crystallinity of polypyrrole increases in SHI irradiation and is proportionate to ion fluence. The capacitance of the irradiated films is lowered but the capacitance of the supercapacitors with irradiated films showed enhanced stability compared to the devices with unirradiated films while characterized for cycle life up to 10,000 cycles.     

Pumping experiment of water on B and LaB6 films with an electron beam evaporator

The pumping characteristic of water vapor on boron and lanthanum hexaboride films formed with an electron beam evaporator have been investigated in high vacuum between 10⁻⁴ and 10⁻³ Pa. The measured initial maximum pumping speeds of water for the fresh B or LaB₆ films with a deposition amount from 2.3 × 10²¹ to 6.7× 10²¹ molecules/m² separately formed on a substrate are 3.2–4.9 m³/sm², and the saturation values of adsorbed water on these films are 2.1 ×10²⁰−1.3 × 10²¹ H₂O molecules/m².     

Research of Si and GaAs diode structures by Ion Beam Induced Charge (IBIC) collection

A Si pn junction diode and a GaAs Schottky diode were prepared for studying the basic mechanism of charge collection followed by high energy charged particle incidence in order to improve the resistance against single event upset. A 2 μm wide and 20 μm long rectangular Al electrode attached to a circular Al electrode with a 50 μm diameter was made on a 2.5 μm thick epilayer (minority carrier density 2 × 10¹⁵ /cm³). Both a Schottky electrode of Al (5 μm × 110 μm) and two ohmic electrodes of AuGe/Ni (110 μm × 110 μm) were made on a 2 μm thick epilayer (7.3 × 10¹⁵ /cm³) grown on a semi insulator GaAs substrate (1 × 10⁷ Ω cm). The internal device structure was examined by the IBIC (Ion Beam Induced Charge) method using a 2 MeV He⁺ ion microbeam. IBIC images clearly show an Al electrode, the SiO₂, and an epilayer. These results were then used to improve the qualities of the test diodes.     

Isothermal release of tritium from neutron-irradiated Li17Pb83

Isothermal release experiments were carried out to study the tritium recovery from lithium-lead alloy Li₁₇Pb₈₃ in which tritium was produced by irradiation with thermal neutrons. The experimental results indicate that the tritium recovery was incomplete within two hours at 200 °C. At temperatures above the melting point, the tritium release rates have been significantly increased and found to be controlled by the diffusion in the alloy. The determined diffusion coefficients of tritium in the alloy are 6.6 × 10⁻⁶, 7.8 × 10⁻⁶ and 9.5 × 10⁻⁶ cm²/s at 300, 400 and 500°C, respectively.     

Irradiation growth in deformed zirconium

Single crystals and polycrystals of pure zirconium were irradiated at 353 K and 553 K with fast neutrons to fluences up to 8.1 × 10²⁵ n/m² to determine the effects of various deformation-induced defect structures on irradiation growth. An a-axis single crystal that was swaged 18% grew linearly at a very high rate (˜1.4 × 10⁻²⁸ m²/n) as a result of the massive aligned twins and dislocations (with a-type and c-component Burgers vectors) introduced by deformation. Annealing the swaged crystal at 673 K for 1 h prior to irradiation resulted in a much lower growth rate due to the recovery of the dislocation structure generated by deformation. Annealing the swaged crystal at 823 K instead also retarded growth but to a lesser extent. Grain boundaries, caused by partial recrystallization, were found in the 823 K specimen only and were believed to be responsible for the observed effect. An a-axis crystal that was strained 5% in tension showed little change in length, suggesting that the effect of a small increase in a-type dislocations is relatively minor. Growth was suppressed in the polycrystalline zirconium specimens that were pulled 5%. This is attributed to radiation-enhanced stress relaxation. It also confirms that a high dislocation density is essential to giving a high growth rate in zirconium.     

Heavy-ion-induced luminescence of amorphous SiO2 during nanoparticle formation

Silica glass was implanted with negative 60 keV Cu ions at an ion flux from 5 to 75 μA/cm² up to a fluence of 1 × 10¹⁷ ions/cm² at initial sample temperatures of 300, 573 and 773 K. Spectra of ion-induced photon emission (IIPE) were collected in situ in the range from 250 to 850 nm. Optical absorption spectra of implanted specimens were ex situ measured in the range from 190 to 2500 nm.

IIPE spectra showed a broad band centered around 560 nm (2.2 eV) that was assigned to Cu⁺ solutes. The band appeared at the onset of irradiation, increased in intensity up to a fluence of about 5 × 10¹⁵ ions/cm² and then gradually decreased indicating three stage of the ion beam synthesis of nanoclusters: accumulation of implants, nucleation and growth nanoclusters. The IIPE intensity normalized on the ion flux is independent on the ion flux below 20 μA/cm²at higher fluences. The intensity of the band increased with increasing samples temperature, when optical absorption spectra reveal the increase of Cu nanoparticles size.     

Thermal stability and brazing characteristics of Zr0.7−xMxBe0.3 (M=Ti or Nb) ternary amorphous filler metals

The effects of Ti or Nb substitution on the thermal stability and brazing characteristics of Zr_0.7−xM_xBe_0.3 (M=Ti or Nb) ternary amorphous alloys were investigated in order to improve properties of Zr–Be binary amorphous alloy as a new filler metal for joining zirconium alloy. The Zr_0.7−xM_xBe_0.3 (M=Ti or Nb; 0x0.1) ternary amorphous alloys were produced by melt-spinning method. In the selected compositional range, the thermal stability of Zr_0.7−xTi_xBe_0.3 and Zr_0.7−xNb_xBe_0.3 amorphous alloys are improved by the substitution of titanium or niobium for zirconium. As the Ti and Nb content increases, the crystallization temperatures increase from 610°C to 717°C and 610°C to 678°C, respectively. These amorphous alloys were put into practical use in joining bearing pads on zircaloy cladding sheath. Using Zr–Ti–Be amorphous alloys as filler metals, smooth interface and spherical primary particles (proeutectic phase) appear in the brazed layer, which is the similar microstructure of using Zr_0.7Be_0.3 binary amorphous alloys. In the case of Zr–Nb–Be amorphous alloys, Ni-precipitated Zr phase that may cause some degradation in ductility and corrosion-resistance is formed at both sides of the brazed layer.     

Depth profiling study on the migration of tritium in titanium induced by deuterium-ion bombardment

A thin titanium layer with uniformly absorbed tritium (T/Ti ˜1.0) was bombarded by 390 keV D₃⁺ ions (130 keV per deuteron). Bombardment was performed at low (111 K) and room temperatures up to fluences of 5.9 × 10¹⁸ D/cm² and 3.0 × 10¹⁸ D/cm², respectively. Depth profiles of tritium up to a depth of 0.8 mg/cm² (˜1.8 μm) were measured and the change of the profile with fluence was investigated by means of the T(d, )n nuclear reaction. At both of the temperatures, a dip was formed on the depth profile of tritium at the depth around the projected range, indicating that the deuteron bombardment induced the migration of tritium against the concentration gradient. At the low temperature, the dip showed a gradual growth with fluence and saturation of the growth at the higher fluences, which could not be described by the existing model for isotope mixing. The spectrum of protons from the D(d, p)T reaction obtained in the same measurement suggested that the release of deuterium suddenly started at the final stage of the present bombardment. The dip formed at room temperature was larger than that at the low temperature. The migration of tritium induced by the bombardment is discussed on the basis of the experimental results obtained.     

Electronic excitation effects in CeO2 under irradiations with high-energy ions of typical fission products

In order to understand the formation mechanism of a crystallographic re-structuring in the periphery region of high-burnup nuclear fuel pellets, named as “rim structure”, information on the accumulation process of radiation damage and fission products (FPs), as well as high-density electronic excitation effects by FPs, are needed. In order to separate each of these processes and understand the high-density electronic excitation effects, 70–210 MeV FP ion (Xe^10–14+, I⁷⁺ and Zr⁹⁺) irradiation studies on CeO₂, as a simulation of fluorite ceramics of UO₂, have been done at a tandem accelerator of JAEA-Tokai and the microstructure changes were determined by transmission electron microscope (TEM). Measurements of the diameter of ion tracks, which are caused by high-density electronic excitation, have clarified that the effective area of electronic excitation by high-energy fission products is around 5–7 nm  and the square of the track diameter tends to follow linear function of the electronic stopping power (S_e). Prominent changes are hardly observed in the microstructure up to 400 °C. After overlapping of ion tracks, the elliptical deformation of diffraction spots is observed, but the diffraction spots are maintained at higher fluence. These results indicate that the structure of CeO₂ is still crystalline and not amorphous. Under ion tracks overlapping heavily (>1 × 10¹⁵ ions/cm²), surface roughness, with characteristic size of the roughness around 1 μm, is observed and similar surface roughness has also been observed in light-water reactor (LWR) fuels.     

Investigation of the radiation hardness on semiconductor devices using the ion micro-beam

Variation of the ion beam induced charge (IBIC) pulse heights due to ion irradiation was investigated on a Si pn diode and a 6H-SiC Schottky diode using a 2 Mev He⁺ micro-beam. Each diode was irradiated with a focused 2 MeV He⁺ micro-beam to a fluence in the range of 1×10⁹–1×10¹³ ions/cm². Charge pulse heights were analyzed as a function of the irradiation fluence. After a 2 MeV ion irradiation to the Si pn junction diode, the IBIC pulse height decreased by 15% at 9.2×10¹² ions/cm². For the SiC Schottky diode, with a fluence of 6.5×10¹² ions/cm², the IBIC pulse height decreased by 49%. Our results show that the IBIC method is applicable to evaluate irradiation damage of Si and SiC devices and has revealed differences in the radiation hardness of devices dependent on both structural and material.     

Real-time evolution of ion–surface interactions of MgAl2O3 and LiNbO3 detected by ion-induced photon spectroscopy

Ion-induced photon emission under 60 keV Cu⁻ implantation into the insulators of MgAl₂O₄ and LiNbO₃ was in situ measured over a wide wavelength range from 200 to 900 nm. The formation of the Mg and Li deficient layers for the respective insulator was detected based on the dose dependence of the Al, Mg and Li atomic line intensities. The Al I and Mg I line intensities from spinel exhibit different behaviors depending on irradiation temperatures: they gradually decrease while the (Al I)/(Mg I) ratio increases up to dose of 3×10¹⁷ ions/cm² at room temperature or exhibits a steady-state tendency at high temperature. Sharp decrease of Li I line intensity from LiNbO₃ under high dose rate bombardment indicates drastic changes of surface layer that may alter the phase stability and optical performance of insulators.