Characterization of swift heavy ion tracks in CaF2 by scanning force and transmission electron microscopy

Single crystals of fluorite (CaF₂) were exposed to various swift heavy ions (Ca up to U) of energy 1–11.1 MeV per nucleon, covering a large range of electronic stopping power S_e between 4.6 and 35.5 keV/nm. The irradiated (1 1 1) cleaved surfaces were investigated by means of scanning force microscopy in tapping mode. Nanometric hillocks produced by the ion projectiles were analyzed in terms of creation efficiency E_eff, diameter and height values, and diameter–height correlation. Hillock formation appears with a low efficiency above a S_e threshold of 5 keV/nm. The mean height of these hillocks is approximately constant (1 nm) between 5 and 10 keV/nm and increases linearly with S_e above 10 keV/nm reaching 12.5 nm for the largest S_e value investigated. Similarly, the efficiency grows versus S_e achieving 100% for S_e > 13 keV/nm where each projectile produces an individual hillock. Above 13 keV/nm, the hillock height and diameter are strongly correlated. The diameter was deduced by graphical deconvolution of the scanning-tip curvature that is determined experimentally for each set of measurements. In the entire S_e regime, the mean diameter exhibits a constant value of 13 nm, which is significantly larger than 6 nm wide tracks observed by transmission electron microscopy.     

Neutron yields from 1 GeV/nucleon U ion beams on Fe target

Yields of neutrons produced by a ²³⁸U ion beam of 1 GeV/nucleon kinetic energy impinging on a thick Fe target were measured resulting in distributions differential in neutron angle (0° < _n < 20°) and in kinetic energy (T_n > 50 MeV). The data serve in radiation protection planning for next-generation rare-isotope beam facilities. The experimental data are contrasted with predictions from transport codes as currently used in radiation shield design studies.     

Superconductivity in MgB2 films synthesized by ablation from high-power ion beam

MgB₂ thin films with T_c = 19 K were fabricated by the ion ablation technique utilizing a high-energy pulsed ion beam. A target remains pure MgB₂ after ablation, proving the excellent capability of ablation by the high-power ion beam. Chemical compositions of the deposited material, however, may vary with positions of the substrates from the beam axis. X-ray diffraction patterns exhibit only (0 0 1) and (0 0 2) peaks, which indicate a c-axis orientation of the films. Scanning electron microscopy images show a possible growth of single crystals with hexagonal shape and 1 μm size.     

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.     

Interface mixing induced by swift heavy ions at metal-oxide/silicon interfaces

It was observed previously that ceramic/ceramic bilayers were very sensitive with respect to the electronic stopping power S_e, i.e. strong interface mixing, scaling with , occurred if a threshold S_ec was exceeded. The threshold seemed to be determined by the higher track formation threshold of two constituents forming the bilayer. Although no track formation has been observed in crystalline Si even for Uranium projectiles, interface mixing was observed previously for some Si-multilayers.

In this paper we report on the interface mixing of NiO, Fe₂O₃, TiO₂ on Si due to irradiation with 90–350 MeV Ar-, Kr-, Xe- and Au-ions at 80 K at fluences up to 9E15 ions/cm². Interface mixing, analyzed by means of Rutherford Backscattering Spectrometry (RBS), is found for these bilayers, too. But the threshold for intermixing is significantly higher compared to the ceramic/ceramic bilayers. This observation could be an evidence for the threshold being determined by the Si-layer. In contrast to NiO/Si and Fe₂O₃/Si, where an usual random walk mixing Δσ² = kΦ was observed, the interface broadening Δσ² for TiO₂/Si is found to scale nonlinearly with the ion fluence, which indicates that mixing is driven by a chemical solid-state reaction. At higher fluences plateaus form at the low energy Ni-edge of the RBS spectra. The plateaus indicate phase formation. X-Ray diffraction spectra does not show any evidence for new crystalline phases.     

Planar defects in crystalline silicon caused by self-irradiation

We have analysed by computer simulation the evolution of defects caused by self-irradiation of crystalline silicon (c-Si) at high temperatures. A classical molecular dynamics simulation (MD) was followed by defect analysis using the pixel mapping (PM) method. The incident Si ion energy was 5 keV and the target temperature was set to 1000 K. In the present simulation, we aimed to reproduce experimentally observed {3 1 1} planer defects. So far we did not observe long chain structures towards the 1 1 0 direction, nor remarkable platelet {3 1 1} planar defects. Nevertheless we observed a significant increase of 1 1 0-oriented self-interstitial dimers and a small fraction of linear trimers, which will be the initial stages of 1 1 0-rod formation.     

Ion-induced electron emission – monitoring the structure transitions in graphite

The temperature dependence of ion-induced electron emission yield γ under 30 keV Ar⁺ ion impacts at incidence angles θ = 0−80° under dynamically steady-state conditions has been measured for polygranular graphite POCO-AXF-5Q. The fluencies were 10¹⁸–10¹⁹ ion/cm², the temperatures varied from the room temperature (RT) to 400 °C. The RHEED has shown that same diffraction patterns correspond to a high degree of disorder at RT. At high temperature (HT), some patterns have been found similar to those for the initial graphite surfaces. The dependence γ(T) has been found to be non-monotonic and for normal and near normal ion incidence manifests a step-like increase typical for a radiation induced phase transition. At oblique and grazing incidence (θ > 30°), a broad peak was found at T_p = 100 °C. An analysis based on the theory of kinetic ion-induced electron emission connects the behavior of γ(θ,T) to the dependence of both secondary electron path length λ and primary ion ionizing path length R_e on lattice structure that drastically changes due to damage annealing.     

Insight in the outside: New applications of low-energy ion scattering

Low energy ion scattering is used to selectively probe the outermost atomic layer of the surface. The development of double toroidal analyzers has improved the detection sensitivity of low energy ion scattering by orders of magnitude. The features of these analyzers are discussed. It is shown that the absence of matrix effects makes it possible to quantify the surface density of fluorine in polymers with a LiF(1 0 0) surface. The extreme surface sensitivity of LEIS also enables one to study intramolecular segregation processes. As an example the aging of a polypropylene surface that has been activated with atomic oxygen is described. As an example of the LEIS analysis of highly dispersed isolating surfaces, the formation of coke on a commercial three-way catalyst is discussed.     

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.     

Structural evolution in Fe ion implanted Si upon thermal annealing

We have performed high-dose Fe ion implantation into Si and characterized ion-beam-induced microstructures as well as annealing-induced ones using transmission electron microscopy (TEM) and grazing-incidence X-ray diffraction (GIXRD). Single crystals of Si(1 0 0) substrate were irradiated at 623 K with 120 keV Fe⁺ ions to a fluence of 4 × 10¹⁷ cm⁻². The irradiated samples were then annealed in a vacuum furnace at temperatures ranging from 773 K to 1073 K. Cross-sectional TEM observations and GIXRD measurements revealed that a layered structure is formed in the as-implanted specimen with ε-FeSi, β-FeSi₂ and damaged Si, as component layers. A continuous β-FeSi₂ layer was formed on the topmost layer of the Si substrate after thermal annealing.     

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.     

Influence of ageing heat treatment on alloy A-286 microstructure and stress corrosion cracking behaviour in PWR primary water

The influence of ageing heat treatment on alloy A-286 microstructure and stress corrosion cracking behaviour in simulated Pressurized Water Reactor (PWR) primary water has been investigated. A-286 microstructure was characterized by transmission electron microscopy for ageing heat treatments at 670 °C and 720 °C for durations ranging from 5 h to 100 h. Spherical γ′ phase with mean diameters ranging from 4.6 to 9.6 nm and densities ranging from 8.5 × 10²² m⁻³ to 2 × 10²³ m⁻³ were measured. Results suggest that both the γ′ phase mean diameter and density quickly saturate with time for ageing heat treatment at 720 °C while the γ′ mean diameter increases significantly up to 100 h for ageing heat treatment at 670 °C. Grain boundary η phase precipitates were systematically observed for ageing heat treatment at 720 °C even for short ageing periods. In contrast, no grain boundary η phase precipitates were observed for ageing heat treatments at 670 °C except after 100 h. Hardening by γ′ precipitation was well described by the dispersed barrier hardening model with a γ′ barrier strength of 0.23. Stress corrosion cracking behaviour of A-286 was investigated by means of constant elongation rate tensile tests at 1.5 × 10⁻⁷ s⁻¹ in simulated PWR primary water at 320 °C and 360 °C. In all cases, initiation was transgranular while propagation was intergranular. Grain boundary η phase precipitates were found to have no significant effect on stress corrosion cracking. In contrast, yield strength and to a lesser extent temperature were found to have significant influences on A-286 susceptibility to stress corrosion cracking.     

Electrical and optical properties of Co ion implanted a-Si1 − xCx:H alloys

Low resistivity a-Si_1 − xC_x:H alloy films have been formed by high dose Co⁺ ion implantation. The influence of the carbon content of the films on the resistivity has been studied and the lowest values, of the order of 10 Ω/Sq, have been observed for the carbon free films. Even lower resistivities, a further reduction of up to 50%, have resulted from annealing at temperatures up to 500°C. Changes in the optical and structural properties of the implanted a-Si_1 − xC_x:H films have been studied by means of IR and Raman spectroscopy. Results show that the implantation produces considerable structural and chemical modifications. The formation of, and the transition to, a possible CoSi₂ phase has been observed by examining the IR and Raman spectra as a function of implant dose.     

Effect of annealing on the optical absorption of Ni nanoparticles in MgO single crystals

Ni⁺ ion implantation with an energy of 64 keV in MgO single crystals was conducted at room temperature up to a fluence of 1 × 10¹⁷ ion/cm². The as-implanted crystals were annealed isochronally at temperatures up to 900 °C. Optical absorption spectroscopy, X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) have been utilized to characterize the changes of optical properties and the microstructure of the annealed samples. XPS results showed that the charge state of implanted Ni was still mainly in metallic Ni⁰ after annealing at 900 °C. TEM analysis revealed metallic Ni nanoparticles with depth-dependant dimensions of 1–10 nm in the annealed sample. Optical absorption spectroscopy indicated that the Ni nanoparticles exhibited a broad surface plasmon resonance absorption band in annealed samples and the band shifted to a longer wavelength with the increasing annealing temperature.     

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.     

Enthalpy and heat capacity of LiAlO2 between 298 and 1700 K by drop calorimetry

The enthalpy of γ-LiAlO₂ was measured between 403 and 1673 K by isothermal drop calorimetry. The smoothed enthalpy curve between 298 and 1700 K results in H⁰(T) − H⁰(298 K)=−37 396 + 93.143 · T + 0.00557 · T² + 2 725 221 · T⁻¹ J/mol. The standard deviation is 2.2%. The heat capacity was derived by differentiation of the enthalpy curve. The value extrapolated to 298 K is C_p,298=(65.8 ± 2.0) J/K mol.     

Criticality in the fabrication of ion extraction system for SST-1 neutral beam injector

For the heating of plasma in steady-state superconducting tokamak (SST-1) (Y.C. Saxena, SST-1 Team, Present status of the SST-1 project, Nucl. Fusion 40 (2000) 1069–1082; D. Bora, SST-1 Team, Test results on systems developed for the SST-1 tokamak, Nucl. Fusion 43 (2003) 1748–1758), a neutral beam injector is provided to raise the ion temperature to 1 keV. This injector has a capability of injecting hydrogen beam with the power of 0.5 MW at 30 keV. For the upgrade of SST-1, power of 1.7 MW at 55 KeV is required. Further, beam power is to be provided for a pulse length of 1000S. We have designed a neutral beam injector (S.K. Mattoo, A.K. Chakraborty, U.K. Baruah, P.K. Jayakumar, M. Bandyopadhyay, N. Bisai, Ch. Chakrapani, M.R. Jana, R. Onali, V. Prahlad, P.J. Patel, G.B. Patel, B. Prajapati, N.V.M. Rao, S. Rambabu, C. Rotti, S.K. Sharma, S. Shah, V. Sharma, M.J. Singh, Engineering design of the steady-state neutral beam injector for SST-1, Fusion Eng. Des. 56 (2001) 685–691; A.K. Chakraborty, N. Bisai, M.R. Jana, P.K. Jayakumar, U.K. Baruah, P.J. Patel, K. Rajasekar, S.K. Mattoo, Neutral beam injector for steady-state superconducting tokamak, Fusion Technol. (1996) 657–660; P.K. Jayakumar, M.R. Jana, N. Bisai, M. Bajpai, N.P. Singh, U.K. Baruah, A.K. Chakraborty, M. Bandyopadhyay, C. Chrakrapani, D. Patel, G.B. Patel, P. Patel, V. Prahlad, N.V.M. Rao, C. Rotti, V. Sreedhar, S.K. Mattoo, Engineering issues of a 1000S neutral beam ion source, Fusion Technol. 1 (1998) 419–422) satisfying the requirements for both SST-1 and its upgrade. Since intense power is to be transported to SST-1 situated at a distance of several meters from the ion source, the optical quality of the beam becomes a primary concern. This in turn, is determined by the uniformity of the ion source plasma and the extractor geometry. To obtain the desired optical quality of the beam, stringent tolerances are to be met during the fabrication of ion extractor system.

SST-1 neutral beam injector is based on positive ion source. The extraction system consists of three grids, each having extraction area of (width) 230 mm × (height) 480 mm and 774-shaped apertures of 8-mm diameter. To obtain horizontal focal length of 5.4 m and vertical of 7 m, each grid consists of two halves with 387 apertures. Two halves are inclined at an angle of 1.07 ± 0.01°. For long pulse operation, active water cooling is provided by in-laid down of dense network of 22 wavy semicircular (r = 1.1 ± 0.05 mm) cooling channels in the space available between the apertures. The required flatness of the copper plate is 100 μm and positioning tolerance of aperture is ±60 μm. The measurement obtained after fabrication is compared with the specifications. It is pointed out that fabrication within set tolerance limit could be achieved only through process of fabrication and high-resolution measurements.     

Spin-resolved magnetic studies of focused ion beam etched nano-sized magnetic structures

Scanning ion microscopy with polarization analysis (SIMPA) is used to study the spin-resolved surface magnetic structure of nano-sized magnetic systems. SIMPA is utilized for in situ topographic and spin-resolved magnetic domain imaging as well as for focused ion beam (FIB) etching of desired structures in magnetic or non-magnetic systems. Ultra-thin Co films are deposited on surfaces of Si(1 0 0) substrates, and ultra-thin, tri-layered, bct Fe(1 0 0)/Mn/bct Fe(1 0 0) wedged magnetic structures are deposited on fcc Pd(1 0 0) substrates. SIMPA experiments clearly show that ion-induced electrons emitted from magnetic surfaces exhibit non-zero electron spin polarization (ESP), whereas electrons emitted from non-magnetic surfaces such as Si and Pd exhibit zero ESP, which can be used to calibrate sputtering rates in situ. We report on new, spin-resolved magnetic microstructures, such as magnetic “C” states and magnetic vortices, found at surfaces of FIB patterned magnetic elements. It is found that FIB milling has a negligible effect on surface magnetic domain and domain wall structures. It is demonstrated that SIMPA can evolve into an important and efficient tool to study magnetic domain, domain wall and other structures as well as to perform magnetic depth profiling of magnetic nano-systems to be used in ultra-high density magnetic recording and in magnetic sensors.     

Investigation of metal matrix systems for cosmogenic Al analysis by accelerator mass spectrometry

We report experiments designed to help optimize accelerator mass spectrometry (AMS) of ²⁶Al (in the form of Al₂O₃) for geochronologic and geomorphologic applications. Analysis times are long and the precision of AMS are restricted by counting statistics for ²⁶Al, which are in turn limited by the intensity of Al⁻ beam currents. We show that ion beam currents are affected by the metal matrix in which Al₂O₃ is dispersed, by the matrix-to-Al₂O₃ mixing ratio, and for at least some matrices, such as Ag, by the depth to which the sample is packed in the AMS cathode. Typical instantaneous Al⁺⁷ currents (μA) produced by the LLNL CAMS Cs sputter ion source and measured in a Faraday cup after the accelerator are 2.26 for samples in Ag, 2.17 in Re, 2.00 in Nb, 1.92 in V and 1.73 in Mo. The AMS counting efficiency (Al⁻ ions detected per Al atom loaded in the target) for a constant analysis time (900 s) and for equimolar mixtures of Al₂O₃ and matrix is in the range of 6 × 10⁻⁵–9 × 10⁻⁵ in the order Ag > Re > Nb > V > Mo. Additionally, we observed a correlation between the ion detection efficiency (Al ions detected per Al atoms loaded) and the matrix work function and inverse vaporization enthalpy of the matrix and beam current. Typical currents (μA) obtained with elemental Al are 13.3 for samples in no matrix, 3.23 in V, 3.14 in Nb, 3.07 in Re, 2.85 in Mo, 1.46 in Ag. The ion detection efficiency for elemental Al correlates strongly with matrix electron affinity. Thus, our data indicate that the current practice of mixing Al₂O₃ with Ag is reasonable until a means is found to produce cathodes of elemental Al.     

Carbon ion-implanted optical waveguides in Nd:YLiF4 crystal: Refractive index profiles and thermal stability

We report on the optical planar waveguides in Nd:YLiF₄ laser crystals fabricated by 6.0 MeV C³⁺ ion implantation at doses of 1 × 10¹⁵ or 2.5 × 10¹⁵ ions/cm², respectively. The refractive index profiles, which are reconstructed according to the measured dark mode spectroscopy, show that the ordinary index had a positive change in the surface region, forming non-leaky waveguide structures. The extraordinary index is with a typical barrier-shaped distribution, which may be mainly due to the nuclear energy deposition of the incident ions into the substrate. In order to investigate the thermal stability of the waveguides, the samples are annealed at temperature of 200–300 °C in air. The results show that waveguide produced by higher-dose carbon implantation remains relatively stable with post-irradiation annealing treatment at 200 °C in air.