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.     

X-ray irradiation of ion-implanted MOS capacitors

He⁺ ion-implanted metal-oxide-semiconductor (MOS) capacitors with two different oxide thickness have been irradiated by X-rays and the depth distribution of the implant damage in the Si–SiO₂ structures have been examined. The efficiency of X-ray annealing of electronic traps caused by implantation and changes in charge populations are reported. The experiment shows that (in the case when defects introduced by implantation are located at the Si–SiO₂ interface) only defects corresponding to the deep levels in the Si can be affected by X-ray irradiation. When defects introduced by ion implantation are located deeper within the Si substrate complete annealing of these defects is observed.     

RBS studies of the lattice damage caused by 1 Me V Si implantation into Al0.3Ga0.7As/GaAs superlattices at elevated temperature

The lattice damage accumulation in GaAs and Al_0.3Ga_0.7As/GaAs superlattices by 1 MeV Si⁺irradiation at room temperature and 350°C has been studied. For irradiations at 350°C, at lower doses the samples were almost defect-free after irradiation, while a large density of accumulated defects was induced at a higher dose. The critical dose above which the damage accumulation is more efficient is estimated to be 2 × 10¹⁵ + Si/cm² for GaAs, and is 5 × 10¹⁵ Si/cm² for Al_0.8Ga_0.7As/GaAs superlattice for implantation with 1.0 MeV Si ions at 350°C. The damage accumulation rate for 1 MeV Si ion implantation in Al_0.3Ga_0.7As/GaAs superlattice is less than that in GaAs.     

The effect of alpha-particle and proton irradiation on the electrical and defect properties of n-GaAs

Radiation damage effects were studied in n-GaAs grown by organo-metallic vapour phase epitaxy (OMVPE) for a wide range of alpha-particle (2.0 MeV and 5.4 MeV) and proton (2.0 MeV) particle fluences, using an americium-241 (Am-241) radio-nuclide and a linear Van de Graaff accelerator as the particle sources. The samples were irradiated at 300 K, after fabricating palladium Schottky barrier diodes (SBDs) on the 1.2 × 10¹⁶ cm³ Si-doped epitaxial layers. The irradiation-induced defects are characterized using conventional deep level transient spectroscopy (DLTS). A correlation is made between the change in SBD characteristics and the quantity and type of defects introduced during irradiation. It is shown that the two parameters most susceptible to this irradiation are the reverse leakage current of the SBDs and the free carrier density of the epilayer. The introduction rate and the “signatures” of the alpha-particle and proton irradiation-induced defects are calculated and compared to those of similar defects introduced during electron irradiation.     

Thermal conductivity degradation of ceramic materials due to low temperature, low dose neutron irradiation

The thermal conductivity degradation due to low-temperature neutron irradiation is studied and quantified in terms of thermal resistance terms. Neutron irradiation is assumed to have no effect on umklapp scattering. A theoretical model is presented to quantify the relative phonon-scattering effectiveness of the three dominant defect types produced by neutron irradiation: point defects, dislocation loops and voids. Several commercial ceramics have been irradiated with fission reactor fast neutrons at low temperatures to produce defects. Materials include silicon carbide, sapphire, polycrystalline alumina, aluminum nitride, silicon nitride, beryllium oxide, and a carbon fiber composite. The neutron dose corresponded to 0.001 and 0.01 displacements per atom (dpa) for a 60 °C irradiation and 0.01 and 0.1 dpa for a 300 °C irradiation. Substantial thermal conductivity degradation occurred in all of the materials except BeO following irradiation at 60 °C to a dose of only 0.001 dpa. The data are discussed in terms of the effective increase in thermal resistance caused by the different irradiation conditions. Evidence for significant point defect mobility during irradiation at 60 and 300 °C was obtained for all of the ceramics. The thermal stability of the radiation defects was investigated by isochronal annealing up to 1050 °C.     

Co γ-ray irradiation effects on dielectric characteristics of tin oxide films of different thicknesses on n-type Si(1 1 1) substrates

We have tried to determine the effects of ⁶⁰Co gamma irradiation on properties of Au/SnO₂/n-Si (MOS) structures such as dielectric constant (ε′), dielectric loss (ε″), tangent loss (tan δ) and ac conductivity (σ_ac). Three samples were fabricated with different deposition time. The samples were irradiated using a ⁶⁰Co γ-ray source irradiation with the total dose range of 0–500 kGy at room temperature. Capacitance and conductance (C–G–V) measurements were performed at a frequency of 500 kHz in the dark and at room temperature before and after irradiation. The experimental data were analyzed using complex permittivity and electric modulus. The values of ε′, ε″, tan δ and σ_ac showed a strong dependence on the applied voltage and irradiation dose. The dielectric properties of MOS structures have been found to be strongly influenced by the presence of dominant radiation-induced defects. Experimental results show that the interfacial polarization contributes to the improvement of dielectric properties of Au/SnO₂/n-Si (MOS) Schottky diodes.     

Hydrogen concentration on mirror surfaces of neutron bottles

Concentrations and depth distributions of the surface hydrogen and the surface deuterium in vacuum evaporated nickel layers and beryllium plates have been investigated by the ERDA method. It is shown that if the evaporation vacuum pressure is kept better than 10⁻⁶ Torr, the hydrogen adsorption from the residual gas during the evaporation is negligible and the hydrogen from residual or atmospheric gases after the evaporation is the main source of the surface hydrogen. Commercial beryllium plates are found to have surface hydrogen of about 10¹⁶ atoms cm². Deuterium treated samples, either in D₂ gas or heavy water, do not show more than possibly a partial replacement of hydrogen. The influence of substrates is small if the thickness of the evaporated nickel layer is more than 2000 Å. The measurements are in good agreement with previously published results.     

粉末冶金态铍在北京谱仪束流管中的应用

根据北京谱仪(BESⅢ)束流管对材料物理性能的要求,对几种材料的物理性能进行比较后,选择粉末冶金态铍作为BESⅢ束流管的中心管材料。采用失重法对粉末冶金态铍在1号电火花加工油中的耐腐蚀性能进行研究,结果表明：粉末冶金态铍在1号电火花加工油中具有较好的耐蚀性,其腐蚀速率由初始的4.18×10^-7kg•m^-2•h^－1逐渐变小,并稳定为1.54×10^-7kg•m^-2•h^－1;在束流管10a的设计寿命内,粉末冶金态铍的最大腐蚀深度估算值为19.9μm,该值是BESⅢ束流管中心管最小厚度600μm的3.32%,满足BESⅢ的工程运行要求。     

双束(H~+/e~-)同时辐照对12Cr-ODS钢氧化物稳定性影响

利用氢离子和电子双束(H~+/e~-)对用化学浸润法制备的新型12cr-ODS铁素体钢进行辐照,研究了辐照对12Cr-ODS钢氧化物稳定性的影响.对不同辐照剂量下原位观察辐照区内氧化物形貌的变化过程发现:辐照前和15 dpa辐照后,约10～20nm氧化物的尺寸并没有明显变化,而氧化物周围出现微小高密度空洞并没有影响氧化物的稳定性;当辐照温度升高至823 K时,大尺寸的氧化物Y_2O_3与基体的相界面变得不规则,但氧化物颗粒尺寸并不发生明显变化.实验结果表明:弥散强化相Y_2O_3尺寸稳定,无明显溶解现象.     

High energy oxygen ion induced modifications in lead based perovskite thin films

The lead based ferroelectric PbZr_0.53Ti_0.47O₃ (PZT), (Pb_0.90La_0.10)TiO₃ (PLT10) and (Pb_0.80La_0.20)TiO₃ (PLT20) thin films, prepared by pulsed laser ablation technique, were studied for their response to the 70 MeV oxygen ion irradiation. The dielectric analysis, capacitance–voltage (C–V) and DC leakage current measurements were performed before and after the irradiation to high-energy oxygen ions. The irradiation produced considerable changes in the dielectric, C–V, leakage characteristics and induced some amount of amorphization. The PZT films showed partial recrystallization after a thermal annealing at 400 °C for 10 min. The phase transition temperature [T_c] of PLT20 increased from 115 °C to 120 °C. The DC conductivity measurements showed a shift in the onset of non-linear conduction region. The current density decreased by two orders of magnitude after irradiation. After annealing the irradiated films at a temperature of 400 °C for 10 min, the films partially regained the dielectric and electrical properties. The results are discussed in terms of the irradiation-induced amorphization, the pinning of the ferroelectric domains by trapped charges and the thermal annealing of the defects generated during the irradiation.     

Optical and structural behaviour of Mn implanted sapphire

Sapphire single crystals were implanted at room temperature with 180 keV manganese ions to fluences up to 1.8 × 10¹⁷ cm⁻². The samples were annealed at 1000 °C in oxidizing or reducing atmosphere. Surface damage was observed after implantation of low fluences, the amorphous phase being observed after implantation of 5 × 10¹⁶ cm⁻², as seen by Rutherford backscattering spectroscopy under channelling conditions. Thermal treatments in air annealed most of the implantation related defects and promoted the redistribution of the manganese ions, in a mixed oxide phase. X-ray diffraction studies revealed the presence of MnAl₂O₄. On the contrary, similar heat treatments in vacuum led to enhanced out diffusion of Mn while the matrix remained highly damaged. The analysis of laser induced luminescence performed after implantation showed the presence of an intense red emission.     

Radiation induced carbon complexes in gallium arsenide

Gallium arsenide grown by the metallorganic chemical vapour deposition method and n-doped to various silicon concentrations was irradiated with reactor neutrons (1 MeV equivalent damage in silicon) in the fluence range 0 to 3 × 10¹⁵ cm⁻². Native defects, including carbon which is a residual impurity of the growth method, and those introduced by irradiation, were characterized by photoluminescence (PL) and deep level transient spectroscopy (DLTS). In some samples with fixed doping value, the PL intensity of all the transitions, including that to the carbon impurity increases at low fluence levels before decreasing at high fluence. At higher fluences, the transition to the carbon impurity goes through other maxima. The carbon PL intensity versus fluence curve depends on initial doping. DLTS results reveal the removal of a trap EL12 at low fluences, but the introduction of other traps at higher fluences. The defect introduction rates depend on fluence. We attribute the variation in the carbon PL intensity to an interaction between the defects introduced by the irradiation and the carbon impurity.     

Atomic mixing at metal–oxide interfaces by high energy heavy ions

We study the atomic mixing at metal (Bi or Au)/oxide (SiO₂ or Al₂O₃) interfaces under 150–200 MeV heavy ion irradiation. Irradiation-induced interface mixing state is examined by means of Rutherford backscattering spectrometry (RBS). For Bi/Al₂O₃ interfaces, the heavy ion irradiations induce a strong atomic mixing and the amount of the mixing increases with increasing the electronic stopping power for heavy ions. By comparing the results with that for 3 MeV Si ion irradiation, we conclude that the strong atomic mixing observed at Bi/Al₂O₃ interfaces is attributed to the high-density electronic excitation. On the other hand, for other interfaces (Bi/SiO₂, Au/Al₂O₃ and Au/SiO₂), atomic mixing is rarely observed after the irradiation. The dependence of atomic mixing on combinations of irradiating ions and interface-forming materials is discussed.     

压水堆二回路工况下碱化剂对结构材料腐蚀的影响

利用长期浸泡的方法分析研究了压水堆二回路工况下A508Ⅲ和A106Gr.B低合金钢在乙醇胺（ETA）+二甲胺（DMA）、ETA、氨（NH₃·H₂O） 3种碱化剂中的均匀腐蚀行为,并利用扫描电镜、X射线光电子能谱和AES等技术分析了氧化膜的结构和组分。结果表明,在2 000 h试验后,A508Ⅲ试样在NH₃·H₂O中的腐蚀速率为0.15 mg/(dm²·h),而在ETA+DMA条件下的腐蚀速率为0.087 mg/(dm²·h),较在NH₃·H₂O中降低约42%。对于A106Gr.B材料,ETA+DMA环境的腐蚀速率相对于NH₃·H₂O环境下降约29.01%,说明复合碱化剂条件下,试样更耐蚀。氧化膜结构分析表明,氧化膜主要以Fe和O为主,ETA+DMA环境下的氧化膜厚度较薄,结构更加致密,氧化膜内含有N元素,说明胺分子参与了氧化膜的生成。复合碱化剂下材料耐蚀性提高的主要原因是由于复合碱化剂中的胺挥发性小于NH₃·H₂O,液相冷却剂pH值升高,减缓了Fe的氧化反应,另外胺分子易通过吸附作用吸附于氧化膜表面,降低了金属氧化反应的活化能,提高了材料的耐蚀性能。复合碱化剂与二回路设备材料具有较好的相容性,能有效降低设备材料的腐蚀速率,对于二回路水化学处理方法的改进有积极意义。     

Application of the rapid thermal process: sintering the sputteredaluminum/silicon contact in silicon detector fabrication

Rapid thermal process (RTP) sintering of aluminum metallization has been used in p⁺-n junction detector fabrication. For the same thickness of aluminum film and at the same RTP sintering condition, the leakage current of the p⁺-n junction detectors with sputtered Al metallization showed at least a 50% improvement after sintering, and no spiking phenomena were observed compared to the detectors with evaporated Al contacts. RTP sintering in 4% H₂/N₂ ambient passivates the defects introduced by sputtering and the damage caused by the ⁶⁰Co irradiation     

Electronic energy-density effects in ion tracks of metals

High resolution Auger-electron spectroscopy has been applied to the interaction of swift heavy ions with atomically clean metallic solids. Spectra have been taken for fast projectile electrons and for charge-state equilibrated ions at normal incidence on microcrystalline beryllium samples, Al(1 0 0) single crystals and several metallic glasses (Al₈₇La₇Ni₅Zr₁, Ni₇₈B₁₄Si₈, Co₆₆Si₁₆B₁₂Fe₄Mo₂). From the energy shift and from the Auger-line width we have extracted ion-track potentials and also electron temperatures inside ion tracks. A first determination of the angular distribution of multiple-ionization lines is presented as well.     

Defect evolution during ion bombardment of amorphous Si probed by in situ conductivity measurements

In this work we use in-situ conductivity measurements during ion irradiation as a sensitive probe of the defect structure of amorphous Si. Electronic transport in amorphous Si occurs by hopping at the high density ( 10²⁰ cm⁻³ eV⁻¹) of deep lying localized states introduced by the defects in the band gap. In-situ conductivity measurements allow to follow directly the defect generation and annihilation kinetics during and after ion bombardment of the material. Amorphous Si layers, patterned to perform conductivity measurements, were annealed at 500°C in order to reduce the defect density by about a factor of 5. Defects were subsequently reintroduced by high energy ion irradiation at different temperatures (77–300 K). During irradiation the conductivity of the layer increases by several orders of magnitude and eventually saturates. Turning off the beam results in a decrease of the conductivity by a factor of 2 in times as long as a few hours even at 77 K. The effects of different ions (He, C, Si, Cu, and Au) and different ion fluxes (10⁹–10¹² ions/cm² s) on these phenomena have been explored. These data give a hint on the mechanisms of defect production and annihilation and demonstrate a strong correlation between electrical and structural defects in amorphous silicon.     

Helium-implanted CLAM steel and evolutionary behavior of defects investigated by positron-annihilation spectroscopy

China Low Activation Martensitic (CLAM) steel has been chosen as the primary candidate structural material for the first wall/blanket for fusion reactor. The excessive helium irradiation induced damage of CLAM steel at high temperatures and the evolution of defects were investigated in this paper. The samples were homogeneously implanted with 1e + 17 ions/cm² and 100 keV of helium at room temperature, 473, 673, and 873 K. Irradiation induced damage of CLAM steel and the annealing behavior of defects were probed by slow positron beam Doppler broadening technique. Helium implantation produced a large number of vacancy-type defects which bound with helium and formed helium–vacancy complexes. Target atoms’ displacement capacity was strengthened with rising irradiation temperatures, so the S parameter increased with increasing irradiation temperatures, and helium–vacancy complexes were main defects after helium implantation at damage layers. Helium bubbles would be unstable and the desorption of helium bubbles would promote the density of defects above 673 K. By analyzing the curves of S–W and annealing tests of irradiated specimen, it suggested that there werenot only one type of defect in damage layers. Though helium–vacancy complexes were primary defects after helium implanted, introducing excessive helium might also generated other point defects or dislocation loops in the material.     

Beryllium

The properties and fundamental methods of preparing metallic beryllium are discussed on the basis of results obtained by Soviet authors.Comparison is made between thermal reduction of beryllium fluoride by magnesium, electrolytic extraction, and purification of beryllium by distillation in vacuum.Preparation of beryllium articles by different methods of powder metallurgy, melting in vacuum induction furnaces with centrifugal casting, extrusion of beryllium articles and the structure and properties of compact beryllium are discussed. It is found that the maximum tensile strength of pure beryllium samples extruded from a metal hot-pressed in vacuum is about 20 kg/mm² at 425 C and that at this temperature the samples possess high plasticity (over 20% elongation).     

State of helium in irradiated beryllium

Experimental data are presented on the change of the pycnometric density and unit-cell volume of beryllium irradiated in an SM reactor to neutron fluence 14·10²² cm^–2. The behavior of the unit-cell volume as a function of the neutron fluence is similar to the data for other metals. This and data on the volume change in beryllium oxide, where a large amount of gas is also formed during irradiation, make it possible to evaluate critically the assertion that helium forms a solid substitution solution. It is proposed that helium is confined in small accumulations.