Loop formation by ion irradiation in yttria stabilized zirconia

Yttria stabilized zirconia (YSZ) is a candidate material focused as optical and insulating materials in nuclear reactors. Therefore, it is useful to investigate defect formation during irradiation, in order to assess YSZ resistance to radiation damage. In the present study, in situ transmission electron microscopy (TEM) observations were performed on YSZ during 30 keV Ne⁺ ion irradiation in the temperature range of 723–1123 K (using 100 K intervals). Results revealed that damage evolution morphology depends on irradiation temperature. For irradiations below 1023 K, defect clusters and bubbles were formed simultaneously. On the other hand, at 1123 K, only bubbles were formed in the initial stage of irradiation. Loops formed later following the bubble formation. It was also observed that, in the early stage of irradiation above 923 K, larger bubbles were formed along the loop planes compared with other areas.

TEM observations indicated that dislocation loops formed on three kinds of crystallographic planes: namely, {1 0 0}, {1 1 1} and {1 1 2} planes.     

Radiation effects on MgAl2O4–yttria stabilized ZrO2 composite material irradiated with Ne ions at high temperatures

Spinel (MgAl₂O₄) and yttria stabilized ZrO₂ (YSZ) are candidates for fuel materials for use in nuclear reactors and the optical and insulating materials for fusion reactors. In our previous studies, the amorphization of spinel under 60 keV Xe ion irradiation at RT was observed. On the other hand, amorphization could not be confirmed in YSZ single crystals under the same irradiation conditions. In the present study, the damage evolution process of polycrystalline spinel–YSZ composite materials has been studied by in situ TEM observation during ion irradiation. The irradiation was performed with 30 keV Ne⁺ ions at a flux of 5 × 10¹³ ions cm⁻² s⁻¹ at 923 K and 1473 K, respectively. The observed results revealed a clear difference in morphology of damage depending on irradiation temperature and crystal grains. In the irradiation at 923 K, defect clusters and bubbles were formed homogeneously in YSZ grains. On the other hand, at 1473 K, only bubble formation was observed. The bubbles grew remarkably with increasing ion fluence in both grains. Even though the growth of the bubbles was observed in both grains, the average diameter of grown bubbles in spinel grains was larger than those in YSZ ones. The bubbles tended to form along the grain boundary at both temperatures.     

AFM and STM investigation of carbon nanotubes produced by high energy ion irradiation of graphite

Carbon nanotubes (CNT) were produced by high energy, heavy ion irradiation (215 MeV Ne, 246 MeV Kr, 156 MeV Xe) of graphite. On samples irradiated with Kr and Xe ions large craters were found by atomic force microscopy, these are attributed to sputtering. Frequently one or several CNTs emerge from the craters. Some of the observed CNTs showed a regular vibration pattern. No other carbon based materials, like amorphous carbon or fullerenes were evidenced. Focused ion beam cuts were used to compare CNTs with surface folds on graphite.     

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.     

Swift heavy ion induced magnetic phase transition of Fe–Rh alloy

We report the effects of swift heavy ion irradiation on structure and magnetic properties of Fe–50at.%Rh alloys. The alloys are irradiated with 120–200 MeV heavy ions (Ni, Kr or Xe) at room temperature. Before and after the irradiations, the magnetization and the lattice parameter are measured by using superconducting quantum interference device (SQUID) and X-ray diffractometer (XRD), respectively. The lattice parameter at room temperature increases by about 0.3% and antiferromagnetic–ferromagnetic transition temperature decreases below 5 K by the irradiations. Effects of electronic excitation due to swift heavy ions on the change in magnetic properties and lattice structure are discussed.     

The electrical conductivity of carbon nanotube sheets by ion beam irradiation

A method for improving the electrical conductivity of carbon nanotube (CNT) sheets by ion beam irradiation is reported. CNT sheets prepared by a vacuum filtration method were irradiated by Ar and H ion beams at different temperatures. The electrical conductivity of the irradiated CNT sheets at a temperature of 800 K can be improved. The conductivity improvement can be ascribed to the formation of covalent bond crosslinks between CNTs induced by the ion beam irradiation at the elevated temperature.     

He scattering on a TiO2(1 1 0) surface

We present measurements of energy-losses and neutralisation of helium ions on a TiO₂(1 1 0) surface at low keV energies. Measurements were performed in the 1–4 keV energy range. The target azimuthal orientation dependence of total scattering intensity profiles, energy-losses and probability of electron capture or loss were determined. On the basis of Marlowe simulations it is concluded that ion scattering intensities give indications about defects regarding surface bridging O atoms. Variations in energy losses for different scattering directions are reported. Ion fraction measurements were made using both incident ions and neutrals. Similar ion fractions were found indicating that He is efficiently neutralised and ions result from reionisation. These ion fractions are found to depend on the azimuthal orientation and have a minimum along the main crystallographic directions.     

MD simulation of cluster formation during sputtering

The cluster ejection due to cluster impact on a solid surface is studied through molecular dynamics (MD) simulations. Simulations are performed for Cu cluster impacts on the Cu(1 1 1) surface for cluster energy 100 eV/atom, and for clusters of 6, 13, 28 and 55 atoms. Interatomic interactions are described by the AMLJ–EAM potential. The vibration energy spectrum is independent of the incident cluster size and energy. This comes from the fact that sputtered clusters become stable through the successive fragmentation of nascent large sputtered clusters. The vibration energy spectra for large sputtered clusters have a peak, whose energy corresponds to the melting temperature of Cu. The exponent of the power-law fit of the abundance distribution and the total sputtering yield for the cluster impacts are higher than that for the monatomic ion impacts with the same total energy, where the exponent δ is given by Y_n∝n^δ and Y_n is the yield of sputtered n-atom cluster. The exponent δ follows a unified function of the total sputtering yield, which is a monotonic increase function, and it is nearly equal to δ −3 for larger yield.     

Ion beam enhanced etching of LiNbO3

Single crystals of z- and x-cut LiNbO₃ were irradiated at room temperature and 15 K using He⁺- and Ar⁺-ions with energies of 40 and 350 keV and ion fluences between 5 × 10¹² and 5 × 10¹⁶ cm⁻². The damage formation investigated with Rutherford backscattering spectrometry (RBS) channeling analysis depends on the irradiation temperature as well as the ion species. For instance, He⁺-irradiation of z-cut material at 300 K provokes complete amorphization at 2.0 dpa (displacements per target atom). In contrast, 0.4 dpa is sufficient to amorphize the LiNbO₃ in the case of Ar⁺-irradiation. Irradiation at 15 K reduces the number of displacements per atom necessary for amorphization. To study the etching behavior, 400 nm thick amorphous layers were generated via multiple irradiation with He⁺- and Ar⁺-ions of different energies and fluences. Etching was performed in a 3.6% hydrofluoric (HF) solution at 40 °C. Although the etching rate of the perfect crystal is negligible, that of the amorphized regions amounts to 80 nm min⁻¹. The influence of the ion species, the fluence, the irradiation temperature and subsequent thermal treatment on damage and etching of LiNbO₃ are discussed.     

Effect of GeV-Ion irradiation on magnetic properties of Fe–Ni invar alloys

High-energy ion irradiation was performed using a ring-cyclotron installed at the Institute of Physical and Chemical Research (RIKEN). The incident ions were Ta with the energy of 3.71 GeV, and the fluence was fixed to 5 × 10¹² ions/cm². As a target, three sheets of square plates of Fe–30.2 at.% Ni invar alloys were put one upon another. The shift of the Curie temperature T_C of the first sample was 14 K, while that of the second one was 22 K. Comparing these two, the shift was as large as 46 K in the last sample in which ions stopped in the middle. It was concluded that there are at least two different mechanisms that contribute to the shift of T_C.     

Nucleation and growth of defect clusters in CeO2 irradiated with electrons

Nucleation and growth process of defect clusters in cerium dioxide (CeO₂) with fluorite-type crystal structure has been investigated in situ under electron irradiation by using high voltage transmission electron microscopy. Planar defect clusters were formed with electron irradiation ranging from 200 to 1000 keV at temperatures below 450 K. The defect clusters were determined to be faulted-interstitial type dislocation loops lying on {1 1 1} planes. The growth rate of dislocation loops was found to increase with decreasing electron energy. An analysis of the fluence dependence of the growth process of dislocation loops suggests an increase in the vacancy mobility with decreasing electron energy. The rate of the electronic excitation is discussed in terms of the radiation-induced diffusion of oxygen-ion vacancies.     

Temperature dependence of the chemical sputtering of amorphous hydrogenated carbon films by hydrogen

The temperature dependence of chemical erosion and chemical sputtering of amorphous hydrogenated carbon films due to exposure to hydrogen atoms (H⁰) alone and combined exposure to argon ions and H⁰ was measured in the temperature range from 110 to 950 K. The chemical erosion yield for H⁰ alone is below the detection limit for temperatures below about 340 K. It increases strongly with increasing temperature, goes through a maximum around 650–700 K and decreases again for higher temperatures. Combined exposure to Ar⁺ and H⁰ results in substantial chemical sputtering yields in the temperature range below 340 K. In this range the yield does not depend on temperature, but it increases with energy from about 1 (eroded carbon atoms per impinging Ar⁺ ion) to about 4 if the ion energy is increased from 50 to 800 eV. For temperatures above 340 K the measured erosion rates show the same temperature dependence as for the H⁰-only case, but they are higher than for H⁰-only. The difference between the Ar⁺ and H⁰ and the H⁰-only cases increases monotonically with increasing ion energy.     

Defect creation caused by the decay of cation excitons and hot electron–hole recombination in wide-gap dielectrics

Insufficient radiation resistance of construction materials is the Achilles heel for thermonuclear energetics. In wide-gap dielectrics, Frenkel defects are created not only because of the knock-out (impact) mechanism but also because of the decay of the electronic excitations formed during the irradiation (i.e. due to nonimpact mechanisms). The processes of the defect creation at the irradiation of highly pure LiF single crystals at 6–8 K by 1–30-keV electrons, X-rays, or synchrotron radiation of 12–70 eV have been investigated. The annealing processes of these defects in a temperature range up to 200 K have been studied as well. In LiF, creation has been revealed for the following: (1) F–H pairs caused by the decay of anion excitons or by the recombination of electrons and holes, (2) F′–H–V_K and F–I–V_K defect groups at the decay of cation excitons (62 eV), or (3) 20-keV electron irradiation. The mechanism of defect creation at the recombination of hot holes and hot electrons has been discussed for -SiO₂ crystals with an energy gap between the subbands of a valence band. One of the possible ways to suppress this mechanism (“luminescent defence”) is doping a material by luminescent impurities able to capture a part of the energy of hot carriers before their relaxation and recombination (e.g. in MgO:Cr).     

Influence of SHI irradiation on the formation of buried SiC

Silicon carbide (SiC) precipitates buried in Si(1 0 0) substrates were synthesized by ion implantation of 50 keV and 150 keV C⁺ ions at different fluences. Two sets of samples were subsequently annealed at 850 °C and 1000 °C for 30 min. Fourier transform infrared (FTIR) spectroscopy studies and X-ray diffraction (XRD) analysis confirmed formation of β-SiC precipitates in the samples. Ion irradiation with 100 MeV Ag⁷⁺ ions at room temperature does not induce significant change in the precipitates. It could be interpreted from the FTIR observations that ion irradiation may induce nucleation in Si + C solution created by ion implantation of C in Si. Modifications induced by swift heavy ion irradiation are found to be dependent on implantation energy of C⁺ ions.     

Irradiation effects of swift heavy ions in actinide oxides and actinide nitrides: Structure and optical properties

Actinide oxides have been used as nuclear fuels in the majority of power reactors working in the world and actinide nitrides are under investigation for the fuels of the future fast neutron fission reactors developed in Forum Generation IV. Radiation damage in actinide oxides UO₂, (U_0.92Ce_0.08)O₂, and actinide nitride UN has been characterized after irradiation with swift heavy ions. Fluences up to 3 × 10¹³ ions/cm² of heavy ions (Kr 740 Mev, Cd 1 GeV) available at the CIRIL/GANIL facility were used to simulate irradiation in reactors by fission products and by neutrons. The macroscopic effects of irradiation remains very weak compared with those seen in other ceramic oxides irradiated in the same conditions: practically no swelling can be measured and no change in colour can be observed on the irradiated part of a polished face of sintered disks. The point defects in irradiated actinide compounds have been characterized by optical absorption spectroscopy in the UV–Vis–NIR wavelength range. The absorption spectra before and after irradiation are compared, and unexpected stability of optical properties during irradiation is shown. This result confirms the low rate of formation of point defects in actinide oxides and actinide nitrides under irradiation. Actinide oxides and nitrides studied are >40% ionic, and oxidation state of the actinides seems to be stable during irradiation. The small amount of point defects produced by radiation (<10¹⁶ cm⁻²) has been identified from differences between the absorption spectrum before irradiation and the one after irradiation: point defects in oxygen or nitrogen lattices can be observed respectively in oxides and nitrides (F centres), and small amounts of U⁵⁺ would be present in all compounds.     

H、He离子辐照对国产ZIRLO合金氧化膜的影响

针对国产ZIRLO合金开展了H、He离子辐照对其腐蚀性能影响的研究。对国产ZIRLO合金样品分别进行高温（300 ℃）H、He离子辐照试验,辐照峰值剂量为1 dpa,之后进行模拟一回路腐蚀试验。通过腐蚀增重方法得到腐蚀动力学曲线。利用慢正电子湮没多普勒展宽谱对未辐照样品和辐照样品进行微观结构表征,用透射电子显微镜对腐蚀125 d的样品进行微观结构表征。结果表明,H、He离子辐照并未改变ZIRLO合金的腐蚀机理。He离子辐照产生的空位团可促进腐蚀过程中裂纹形核,增加了氧扩散通道,减少氧扩散激活能,导致腐蚀初期有明显的加速效应。H离子辐照对腐蚀的加速现象不如He离子辐照明显,原因是H离子辐照产生H-空位复合缺陷对氧扩散激活能减少作用较小。     

注氘低活化马氏体钢在电子辐照下的缺陷行为

低活化铁素体/马氏体(RAFM)钢被视为国际热核聚变反应堆以及聚变反应堆的第1壁候选结构材料之一,很多国家均在研究不同的RAFM钢,中国低活化马氏体(CLAM)钢的研究亦正在进行。核聚变会产生氢、氦、氘及氚,这些气体元素与辐照缺陷结合在一起,对材料的辐照性能会产生较大影响。本文对注氘后不同温度下的辐照后微观结构进行研究。试验利用日本北海道大学的JEOL-1300高压电子显微镜研究注氘CLAM钢从室温到873K在1250keV电子辐照下的微观结构变化。研究结果表明,在电子辐照下,注氘产生的缺陷团会出现消失和长大两种现象,意味着间隙型与空位型位错环在注氘过程中同时产生。并研究了注氘产生的空洞。     

Analysis of molecular oxygen formation in irradiated glasses: a Raman depth profile study

Depth profiles experiments have been performed by Raman spectroscopy on three alkali (Na, Li, K) borosilicate glasses irradiated with 1.8 MeV electrons at 1 and 3 GGy. These experiments show that molecular oxygen produced under β irradiation is concentrated near the glass surface according to a depth depending on the irradiation dose. Moreover, we observed that the polymerisation increase is the same in the entire volume sample. The average Si–O–Si angle decrease under irradiation is also homogeneous in the whole irradiated glass volume. From all results, we demonstrate that oxygen migrates up to the glass surface during irradiation without strong interaction with the glass network. Migration of oxygen and probably alkalis takes place through percolation channels with a possible departure of oxygen in some cases.     

Simulation of ion beam induced crystallization and amorphization in (0 0 1) silicon

The ion beam induced epitaxial crystallization (IBIEC) and the ion beam induced interfacial amorphization (IBIIA) in (0 0 1) silicon caused by 3 MeV Si⁺ and 3 MeV Au⁺ irradiation at 293 K and 623 K are investigated by using a combination of binary collision MC simulations and MD simulations. The energy and angular distribution of the primary recoils is calculated by TRIM and the subcascades caused by the primary recoils are treated by classical MD simulations using a correspondingly large MD cell with 49152 atoms. The resulting topological interface structure is analyzed and compared with that obtained by thermally activated solid phase epitaxy. The rates of crystallization and amorphization are calculated and compared with experimental data. Especially, their dependence on the nuclear deposited energy is discussed.