Determination of sulphur and copper depth distribution in patina layers using nuclear reaction techniques

A method for Cu and S profiling in patina layers was developed by applying a combination of nuclear reaction analysis (NRA) and Rutherford backscattering spectroscopy (RBS). The copper profiling was performed by using the 1327 keV γ-ray deexciting the third excited state to the ground state of ⁶³Cu produced by the reaction ⁶³Cu(p,p^′γ)⁶³Cu. For the determination of sulphur the 2230 keV γ-ray was used deexciting the first excited state to the ground state of ³²S formed through the reaction ³²S(p,p^′γ)³²S, which exhibits three sharp resonances at projectile energies 3.094, 3.195 and 3.379 MeV. The relevant cross-sections were measured in the energy range between 3.0 and 3.7 MeV in steps of 20 keV at 125° to the incident proton beam direction. The technique was tested using artificially produced and natural copper patina layers. Supporting information on the depth distribution of the constituent elements of the patina samples was obtained by p-RBS (E_p: 1.5 MeV, θ: 160°).     

钽靶托在64Cu核素制备工艺中的应用

为了获得适用于⁶⁴Cu核素生产的靶托材料,解决采用铜靶托时氯化铜［⁶⁴Cu］最终产品中非放射性铜杂质含量易超标的问题,获得满足放射性标记要求的氯化铜［⁶⁴Cu］溶液,选用金属钽作为靶托材料,对钽靶托进行热流固耦合分析、镀镍、溶解、辐照以及坠落、热冲击等实验研究,利用钽靶托进行⁶⁴Cu核素的实际生产。结果表明,钽靶托可应用于⁶⁴Cu核素制备,并可简化⁶⁴Cu核素生产工艺,产能可达38.1 GBq(EOB),产额可达190.5 MBq·μA^-1·h^-1(EOB)。所得氯化铜［⁶⁴Cu］溶液的放射性核纯度＞99.9%,放化纯度＞95%,金属杂质含量均低于1.5 μg·GBq^-1。本研究验证了钽靶托可应用于⁶⁴Cu核素生产,避免了镀金工艺,可更高效地进行⁶⁴Cu生产。     

Analysis of Cu and O in high-Tc superconductors by 7–9 MeV protons

The use of proton-induced γ-ray emission for the simultaneous analysis of Cu and O in high-T_c superconductors is demonstrated. Utilizing 7–9 MeV protons, the ratio of O relative to Cu can be determined reliably to a few percent accuracy in homogeneous bulk samples and films thicker than 130 μm using standard bulk samples of O and Cu. Results of the present method are compared with those of the analysis of YBa₂Cu₃O_7xdone by the Rutherford scattering of particles and the non-Rutherford scattering through the ¹⁶O(p,p₀)¹⁶O reaction.     

基于C30加速器的64Cu核素制备工艺

64Cu是目前应用十分广泛的放射性核素,主要用于PET诊断。本文基于C30加速器对⁶⁴Cu核素的制备工艺进行研究。制靶靶片为金属铜材质,在靶片表面镀金膜,以保护铜基底。镀金完成后用HCl和H₂O₂浸泡镀金层以去除金属杂质,用脉冲电镀法电镀富集⁶⁴Ni层。将靶片转移至C30加速器固体靶站进行辐照,束流能量为15.5 MeV。将辐照后的靶片转移至分离纯化热室。在溶靶槽中加入6 mol/L HCl和30%H2O2溶靶,使用AG1-X8阴离子交换树脂分离纯化,最终获得⁶⁴Cu核素。分别测定64Cu的放射性核纯度、放射化学纯度、金属杂质含量等质量指标。待收集的64Ni溶液衰变完全后,使用AG1-X8树脂回收。检验结果显示,富集64Ni厚度约8.5～16.3 mg/cm²,⁶⁴Cu产能大于37 GBq,产额可达180～250 MBq/(μA·h),放射性核纯度大于99.9%,放射化学纯度大于97.0%,金属杂质含量均小于0.5 μg/GBq。⁶⁴Cu制备工艺稳定、质量可控,达到了规模化生产水平,为⁶⁴Cu相关药物的研究与开发提供了稳定可靠的核素来源。     

Optical nonlinearity of Cu:SrTiO3 composite fabricated by negative ion implantation

Optical nonlinearity and dispersion were studied for Cu nanoparticle composite. Negative Cu⁻ ions with 60 keV were applied for implanting into SrTiO₃ at a flux of 10 μA/cm² up to a total fluence of 1 × 10¹⁷ ions/cm². The steady-state optical spectrum of Cu-implanted SrTiO₃ showed a surface plasmon resonance resulting from the formation of nanoparticles. Transient transmission and reflection were measured by the pump–probe method with a femtosecond laser system. Optical nonlinearity originated from Cu:SrTiO₃ nanoparticle composite and from SrTiO₃ matrix overlap, in measured transient spectra. The nonlinear component of Cu:SrTiO₃ composite was extracted from the transient spectra with the difference of time response. Nonlinear dielectric coefficient and dispersion around the surface plasmon resonance were derived from extracted transient spectra. The dispersion was compared with a local electric field factor.     

Magnetic force microscopy studies on the magnetic ordering in organic materials induced by high-energy proton irradiation

In this study, ferromagnetic microstructures in highly oriented pyrolytic graphite and superparamagnetic spots in polyimide foils were created by 2.25 MeV proton microbeam irradiation and characterized using atomic and magnetic force microscopy. For this purpose, graphite samples were irradiated with cross-like patterns of 15 μm × 15 μm size using ion fluences in the range of (0.003–2.5) × 10¹⁸ cm⁻². The irradiated crosses showed strong magnetic signals and a complex domain structure in the magnetic images depending on the geometrical dimensions of the crosses. Furthermore, polyimide foils were irradiated with microspots and fluences in the range of (0.016–3.1) × 10¹⁹ cm⁻². Magnetic force microscopy shows very strong phase shifts in these irradiated areas.     

2 MeV Si ion implantation damage in relaxed Si1−xGex

The damage produced by implanting, at room temperature, 3 μm thick relaxed Si_1−xGe_x layers with 2 MeV Si⁺ ions has been measured as a function of Ge content (x = 0.04, 0.13, 0.24 or 0.36) and Si dose in the dose range 10¹⁰–10¹⁵ cm⁻². The accumulation of damage with increasing dose has been studied as a function of Ge content by Rutherford Backscattering Spectrometry, Optical Reflectivity Depth Profiling and Transmission Electron Microscopy and an increased damage efficiency in Si_1−xGe_x with increasing x is observed. The characteristics of implantation-induced defects have been investigated by Electron Paramagnetic Resonance. The results are discussed in the context of a model of the damage process in SiGe.     

Hydrogen dynamics in electrochromic multilayer systems investigated by the N technique

The resonant reaction ¹H(¹⁵N, γ)¹²C was used to determine the depth distribution of hydrogen in two electrochromic multilayer systems. The systems can be bleached and colored by applying an external voltage. To test models explaining this effect by a change of H content (c_H) in electrochromic layers, H profiles of the systems were measured as a function of the applied voltage. For NiO_x, c_H was found to vary as predicted, whereas for WO₃, c_H changes were smaller than expected. Additionally, H uptake into the ITO electrode was observed.     

Range distribution of fluorine in F-implanted LiNbO3

Depth profiles of fluorine in ¹⁹F⁺implanted LiNbO³ have been accurately measured using the ₁₉F(p, γ)¹⁶O resonant nuclear reaction at E_R = 872.1 keV, with Γ = 4.2 keV. A proper convolution calculation method was used to extract the true distribution of fluorine from the experimental excitation yield curves. The experimental range distribution parameters, R_p and ΔR_p, were compared with those obtained by Monte Carlo simulation using a computer code developed recently in this group and with results obtained using the TRIM90 code. It shows that the experimental R_p values agree with the Monte Carlo simulation values very well, while the experimental ΔR_p values are larger than those obtained from the simulations. The simulation with our computer code improves the agreement between the experimental and calculated range straggling, ΔR_p.     

Elemental dissolution study of Pu-bearing borosilicate glasses

Single-pass flow-through tests were conducted to study the effects of self-radiation damage from alpha decay on dissolution kinetics of three radiation-aged Pu-bearing (1 mass% PuO₂) borosilicate glasses over a pH interval of 9–12 at 80–88 °C. The chemical compositions of the glasses were identical except the ²³⁹Pu/²³⁸Pu isotopic ratio, which was varied to yield accumulated doses of 1.3 × 10¹⁶, 2.9 × 10¹⁷ and 2.6 × 10¹⁸ -decays/g at the time of testing. Release of Al, B, Cs, Na, Si and U to solution increased with increasing pH, whereas Ca, Pu and Sr were invariant over the pH interval. Average dissolution rates, based on B release, were identical within experimental uncertainty for all three glass compositions and increased from 0.17 ± 0.07 at pH(23 °C) 9 to 10.6 ± 2.7 (g/(m² d¹)) at pH(23 °C) 12. Release rates of Pu were 10²- to 10⁵-fold slower compared to all other elements and were not affected by isotopic composition, self-radiation damage sustained by the glass, or pH. These data demonstrate that self-radiation damage does not affect glass dissolution rates, despite exposure to internal radiation doses for >20 years.     

Neutron irradiation effects in uranium monosulfide

Uranium monosulfide (US) was irradiated to investigate the effects of fission damage. Post-irradiation examinations were done by measuring the electrical resistivity, and partly the magnetic properties, at low temperature. The lattice parameter and the electrical resistivity measured at room temperature just after the irradiations showed an increase starting at a fission dose of 1 × 10¹⁶ fissions/cm³ and attaining a maximum at 3 × 10¹⁶ fissions/cm³. After that, a saturation of both increases persiste until 3 × 10¹⁷ fissions/cm³. The low-temperature electrical resistivity in the magnetic ordered state (ferromagnetic transition, T_c, at about 180 K) increased remarkably, while decreasing drastically in the magnetization, with increasing fission dose, apparently corresponding to the lattice expansion. In addition, the Curie point (T_c) shifted to lower temperatures with accumulating fission damage.     

Cobalt cross sections for 14 MeV neutrons

14 MeV cross sections for the reactions ⁵⁹Co(n,2n) ^58m+gCo, ⁵⁹Co(n,p) ⁵⁹Fe and ⁵⁹Co(n,) ⁵⁶Mn were measured relative to the ⁵⁶Fe(n,p) ⁵⁶Mn reaction employing the activation technique. Accuracies of about 1% were achieved for the (n,) reaction and 2% for the others. The isomeric cross section ratio was measured for the ⁵⁹Co(n,2n) reactions.

Nuclear reactions – ⁵⁹Co(n,2n) ^58m+gCo, ⁵⁹Co(n,p) ⁵⁹Fe, ⁵⁹Co(n,) ⁵⁶Mn, E_n = 14.3, 14.7 MeV: measured activation cross sections relative to ⁵⁶Fe(n,p) ⁵⁶Mn.

⁵⁹Co(n,2n) ^58m,gCo, E_n = 14.3 MeV; measured isomeric cross section ratio. Natural targets. Ge, NaI and 4πβ detectors.     

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.     

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.     

The diffusivities of fission-created or thermally-doped tritium in UO2

The diffusion behavior of tritium in UO₂ was studied. Two methods were adopted for the introduction of tntium into UO₂: one via ternary fission of ²³⁵U and the other via thermal doping. In the former, the diffusion constants decreased with increase in sample weight. The diffusion constants obtained from the pellet with the same specification (9 mm in diameter, 5 mm high) were D″_bulk = 3.03 × 10⁻³(^+0.369_−0.003) exp[−163±43(kJ/mol)/RT](cm²/s) for fission-created tritium and D′_bulk = 0.15(^{+ 0.94}_−0.13) exp[−76±13 (kJ/mol)/RT](cm²/s) for thermally-doped tritium. The difference of the diffusion constants between two systems was discussed in terms of the effects associated with the recoil processes of energetic tritium.     

Magnetic ordering in superconducting YBa2(Cu1−xFex)3Oy oxide

Magnetic susceptibility measurement and the zero-field muon-spin-relaxation experiment have been made for the YBa₂(Cu_1−xFe_x)₃O_y system. The susceptibility has been measured in the field strong enough for the magnetic flux to penetrate the superconductor and the resultant temperature dependence has demonstrated the field cooled effect and a cusp at low temperatures below T_c. The cusp has been observed when the high field has been applied. The dynamical depolarization rate of the muon obtained by the muon-spin-relaxation experiment has shown the maximum at the same temperature as the cusp. The results suggest that the spin glass freezing of localized magnetic moment takes place at the temperature of the cusp, which is consistent with the previous Mössbauer effect experiments. The magnetic phase diagram for the system has been 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.     

A comparative EPR study of ion implantation induced damage in Si, Si1−xGex (x ≠ 0) and SiC

Electron Paramagnetic Resonance (EPR) measurements have been made to investigate the build up of damage in silicon in relaxed crystalline Si_1−xGe_x (x = 0.04, 0.13, 0.24, 0.36) and in 6H-SiC as a result of increasing the ion dose from low levels (10¹² cm⁻²) up to values (10¹⁵ cm⁻²) sufficient to produce an amorphous layer. Si, Si_1−xGe_x (x ≠ 0) and SiC were implanted at room temperature with 1.5 MeV Si, 2 MeV Si and 0.2 MeV Ge ions respectively. A comparison is made between the ways in which the type and population of paramagnetic defects depend on ion dose for each material.     

Measurement of the H2-D mass difference with a nuclear microprobe

A 1.24 MeV deuteron (D) beam mixed with a H₂ molecular beam was separated with a microslit system of a nuclear microprobe consisting of a 100 μm diameter object and a 1 mm diameter aperture diaphragm. D was distinguished from H₂ by Rutherford backscattering (RBS) on a thin Au film. By slightly changing the magnetic field strength of the beam steerer installed in front of the object diaphragm, the maximum and the minimum RBS D/H₂ ratios were found to be 50.3 and 1.5, respectively. M/ΔM = 3.9 × 10³ was obtained as the mass resolution of the nuclear microprobe. The transmission of this system was 2 × 10⁻³.