Oxygen defects created in CeO2 irradiated with 200 MeV Au ions

CeO₂ films were irradiated with 200 MeV Au ions in order to investigate the damages created by electronic energy deposition. In the Raman spectra of the ion-irradiated films, a broad band appears at the higher frequency side of the F_2g peak of CeO₂. The band intensity increases as ion fluence increases. Furthermore, the F_2g peak becomes asymmetric with a low-frequency tail. In order to understand the origin of these spectral changes, an unirradiated CeO₂ film was annealed in vacuum at 1000 °C. By comparing the results for the irradiation and for the annealing, it is concluded that the broad band obtained for irradiated samples contains the peak observed for the annealed sample. The F_2g peak becomes asymmetric with a low-frequency tail by the irradiation as well as the annealing. Therefore, the above-mentioned changes in the Raman spectra caused by 200 MeV Au irradiation is closely related to the creation of oxygen vacancies.     

Recovery and restructuring induced by fission energy ions in high burnup nuclear fuel

In light water commercial reactors, extensive change of grain structure was found at high burnup ceramic fuels. The mechanism is driven by bombardment of fission energy fragments and studies were conducted by combining accelerator based experiments and computer-science. Specimen of CeO₂ was used as simulation material of fuel ceramics. With swift heavy ion (Xe) irradiation on CeO₂, with 210 MeV, change of valence charge and lattice deviation of cations were observed by XPS and XRD. Combined irradiations of Xe implantation and swift heavy ion irradiation successfully produced sub-micrometer sized sub-grains, similar as that observed in commercial fuels. Studying components of mechanism scenarios, with first principle calculations using the VASP code, we found stable hyper-stoichiometric defect structures of UO_2+x. Molecular dynamics studies revealed stability of Xe planar defects and also found rapid transport mode of oxygen-vacancy clusters.     

Morphological change in FePt nanogranular thin films induced by swift heavy ion irradiation

We have investigated morphology change of FePt nanogranular films (FePt)₄₇(Al₂O₃)₅₃ under irradiation with 210 MeV Xe ions. Here, electron tomography technique was extensively employed to clarify three-dimensional (3D) structure in irradiated specimens, in addition to conventional transmission electron microscopy (TEM) techniques such as bright-field observation and scanning TEM energy dispersive X-ray spectroscopy (STEM-EDX) analysis. The ion irradiation induces the coarsening of FePt nanoparticles with elongation along the beam direction. Electron tomography 3D reconstructed images clearly demonstrated that when the fluence achieves 5.0 × 10¹⁴ ions/cm², well-coarsened FePt balls have been formed on the irradiated surface, and the particles in the film interior have been deformed into rods along the ion trajectory. The alloy particles become inhomogeneous in composition after prolonged irradiation up to 1.0 × 10¹⁵ Xe ions/cm². The particle center is enriched with Pt, while Fe is slightly redistributed to the periphery.     

Effect of Ag and Li ion irradiation on superconducting Tl2Ca2Ba2Cu3O10 single crystals

The effect of irradiation by 50 MeV Li³⁺ and 200 MeV Ag¹⁵⁺ ions on single crystals of Tl₂Ca₂Ba₂Cu₃O₁₀ (Tl2223) superconductor has been investigated at different fluences. Isothermal magnetization hysteresis loops have been recorded at different temperatures using a SQUID magnetometer and the effect of irradiation on the critical current density, irreversible field, second magnetization peak and pinning force has been studied. Irradiation by 200 MeV Ag¹⁵⁺ ions resulted in increased hysteresis and irreversibility field while no change in second magnetization peak position and critical temperature was observed. A broadening in the hysteresis loop before the second magnetization peak was also observed for the crystals irradiated by Li³⁺ ions. Annealing of irradiated crystals at 500 °C resulted in reduction of point defects created by Li³⁺ ions.     

PL and XPS study of radiation damage created by various slow highly charged heavy ions on GaN epitaxial layers

Photoluminescence (PL) spectrum, in conjunction with X-ray photoelectron spectroscopy (XPS) is used to evaluate the surface damage of GaN layer by highly-charged Xe^q+ (18 ? q ? 30), Ar^q+ (6 ? q ? 16) and Pb^q+ (q = 25,35) ions. The intensity of PL emission of GaN layer, including near band-edge peak and yellow luminescence, decreases with increasing fluence and charge state of the incident ions. Finally the PL emission is completely quenched after irradiation to high fluences at high charge state. A new peak at 450 nm appeared in PL spectra of the specimens irradiated with Xe¹⁸⁺, Ar⁶⁺ and Ar¹¹⁺, indicating that radioactive recombination within donor-acceptor pairs (DAPs) during irradiation. After irradiation, XPS spectra show N deficient or Ga rich on GaN surface and XPS spectra of Ga3d core levels indicate spectral peak evidently shifts from a Ga-N to Ga-Ga and Ga-O bond. The relative content of Ga-N bond decreases and the content of Ga-Ga bond increases with the increase of ion fluence and ion charge state. The binding energy of Ga3d_5/2 electron corresponding to Ga-Ga bond of the irradiated GaN film is found to be smaller than that of metallic Gallium (Ga⁰), which can be attributed to irradiation damage.     

Effects of swift heavy ion irradiation on the structure of Er2O3-doped CeO2

In order to simulate the effects of burnable poison doping on the fission fragment damage of UO₂ nuclear fuels, Er₂O₃-doped CeO₂ pellets were irradiated with 200 MeV Xe¹⁴⁺ ions. The irradiation effect was measured by means of X-ray diffraction (XRD). The expansion of lattice and the disordering of atomic arrangement due to the irradiation become more remarkable with increasing the concentration of the Er₂O₃ dopant.     

Amorphisation of ZnAl2O4 spinel under heavy ion irradiation

ZnAl₂O₄ spinels have been irradiated with several ions (Ne, S, Kr and Xe) at the IRRSUD beamline of the GANIL facility, in order to determine irradiation conditions (stopping power, fluence) for amorphisation. We observed by transmission electron microscopy (TEM) that with Xe ions at 92 MeV, individual ion tracks are still crystalline, whereas an amorphisation starts below a fluence of 5 × 10¹² cm⁻² up to a total amorphisation between 1 × 10¹³ and 1 × 10¹⁴ cm⁻². The coexistence of amorphous and crystalline domains in the same pristine grain is clearly visible in the TEM images. All the crystalline domains remain close to the same orientation as the original grain. According to TEM and X-ray Diffraction (XRD) results, the stopping power threshold for amorphisation is between 9 and 12 keV nm⁻¹.     

Color center creation in LiF crystals irradiated with Xe, Kr and N ions: Dependence on fluence and beam current density

Single LiF crystals were irradiated with Xe (195 MeV), Kr (117 MeV), and N (18 MeV) ions. Using absorption spectroscopy, color center creation was analyzed as a function of the ion energy loss, fluence, and flux. The concentration of single F centers and F₂ centers versus fluence and flux exhibits a nonlinear evolution with saturation at higher fluences. For LiF irradiated with N ions at high fluence, the concentration of F centers is proportional to the cube root of the flux indicating the strong interaction of primary hole centers. Macroscopic hillocks were observed in all irradiated LiF crystals by atomic force microscopy.     

Clarification of high density electronic excitation effects on the microstructural evolution in UO2

In order to understand the properties of ion tracks and the microstructural evolution under accumulation of ion tracks in UO₂, 100 MeV Zr¹⁰⁺ and 210 MeV Xe¹⁴⁺ ions irradiation examinations have been done at a tandem accelerator facility of JAEA-Tokai, and it has been observed the microstructure by means of a transmission electron microscope (TEM) and a scanning electron microscope (SEM) in CRIEPI.Comparison of the diameter of ion tracks between UO₂ and CeO₂ under irradiation with 100 MeV Zr¹⁰⁺ and 210 MeV Xe¹⁴⁺ ions at room temperature clarify that the sensitivity on high density electronic excitation of UO₂ is much less than that of CeO₂. By the cross-sectional observation of UO₂ under irradiation with 210 MeV Xe¹⁴⁺ ions at 300 °C, elliptical changes of fabricated pores that exist till ∼6 μm depth and the formation of dislocations have been observed in the ion fluence over 5 × 10¹⁴ ions/cm². The drastic changes of surface morphology and inner structure in UO₂ indicate that the overlapping of ion tracks will cause the point defects, enhance the diffusion of point defects and dislocations, and form the sub-grains at relatively low temperature.     

Effect of swift heavy ion irradiation on nanocrystalline CaS:Bi phosphors: Structural, optical and luminescence studies

Luminescence studies of CaS:Bi nanocrystalline phosphors synthesized by wet chemical co-precipitation method and irradiated with swift heavy ions (i.e. O⁷⁺-ion with 100 MeV and Ag¹⁵⁺-ion with 200 MeV) have been carried out. The samples have been irradiated at different ion fluences in the range 1 × 10¹²-1 × 10¹³ ions/cm². The average grain size of the samples before irradiation was estimated as 35 nm using line broadening of XRD (X-ray diffraction) peaks and TEM (transmission electron microscope) studies. Our results suggest a good structural stability of CaS:Bi against swift heavy ion irradiation. The blue emission band of CaS:Bi³⁺ nanophosphor at 401 nm is from the transition ³P₁ → ¹S₀ of the Bi³⁺. We have observed a decrease in lattice constant (a) and increase of optical energy band gap after ion irradiation. We presume this change due to grain fragmentation by dense electronic excitation induced by swift heavy ion. We have studied the optical and luminescent behavior of the samples by changing the ion energy and also by changing dopant concentration from 0.01 mol% to 0.10 mol%. It has been examined that ion irradiation enhanced the luminescence of the samples.     

Structural studies of Ge nanocrystals embedded in SiO2 matrix

Germanium nanoparticles embedded in SiO₂ matrix were prepared by atom beam sputtering on a p-type Si substrate. The as-deposited films were annealed at temperatures of 973 and 1073 K under Ar + H₂ atmosphere. The as-deposited and annealed films were characterized by Raman, X-ray diffraction and Fourier transform infrared spectroscopy (FTIR). Rutherford backscattering spectrometry was used to quantify the concentration of Ge in the SiO₂ matrix of the composite thin films. The formation of Ge nanoparticles were observed from the enhanced intensity of the Ge mode in the Raman spectra as a function of annealing, the appearance of Ge(3 1 1) peaks in the X-ray diffraction data and the Ge vibrational mode in the FTIR spectra. We have irradiated the films using 100 MeV Au⁸⁺ ions with a fluence of 1 × 10¹³ ions/cm² and subsequently studied them by Raman and FTIR. The results are compared with the ones obtained by annealing.     

Effect of ion beam irradiation on magnetic and structural properties of Pt/Cr/Co multilayers

This paper discusses the effect of ion beam irradiation on the magnetic and structural properties of Pt/Cr/Co multilayers. We observe Co-Cr-Pt ternary alloy phase formation in 1 MeV N⁺ ion irradiated [Pt (2.5 nm)/Cr (0.8 nm)/Co (3.0 nm)]_×6/Si multilayers for a fluence of 1 × 10¹⁶ ions cm⁻² and beyond. The observed phase formation is accompanied by an enhancement in the average grain size, surface roughness and coercivity. Monte Carlo simulation has been performed to study ion-induced defect evolution and atomic displacements to correlate the above observed effects.     

Single- and multiple-electron loss cross-sections for fast heavy ions colliding with neutrals: Semi-classical calculations

Extensive calculations of single, multiple and total electron-loss cross-sections of fast heavy ions in collisions with neutral atoms are performed in the semi-classical approximation using the DEPOSIT code based on the energy deposition model and statistical distributions for ionization probabilities. The results are presented for Ar¹⁺, Ar²⁺, Kr⁷⁺, Xe³⁺, Xe¹⁸⁺, Pb²⁵⁺ and U^q+ (q = 10, 28, 39, 62) ions colliding with H, N, Ne, Ar, Kr, Xe and U atoms at energies E > 1 MeV/u and compared with available experimental data and the n-particle classical-trajectory Monte Carlo (nCTMC) calculations. The results show that the present semi-classical model can be applied for estimation of multiple and total electron-loss cross-sections within accuracies of a factor of 2.From calculated data for the total electron-loss cross-sections σ_tot, their dependencies on relative velocity v, the first ionization potential I₁ of the projectile and the target atomic number Z_A are found and a semi-empirical formula for σ_tot is suggested. The velocity range, where the semi-classical approximation can be used, is discussed.     

Evidence of nanostructure formation in Ge oxide by crystallization induced by swift heavy ion irradiation

Ge oxide films were irradiated with 150 MeV Ag ions at fluences varying between 10¹² and 10¹⁴ ions/cm². The irradiation-induced changes were monitored by FT-IR spectroscopy, atomic force microscopy, X-ray diffraction and photoluminescence spectroscopy. The FT-IR spectra indicate stoichiometric changes and an increase in Ge content on irradiation. X-ray diffraction shows a crystallization of the irradiated films and presence of both Ge and GeO₂ phases. The Ge nanocrystal size, as calculated from Scherrer’s formula, was around 30 nm. The morphological changes, observed in atomic force microscopy, also indicate formation of nanostructures upon ion irradiation and a uniform growth is observed for a fluence of 1 × 10¹⁴ ions/cm².     

Modification of poly(ether ether ketone) by ion irradiation

Poly(ether ether ketone) was irradiated with 3.0 MeV Si²⁺, 3.25 MeV Cu²⁺ and 4.8 MeV Ag²⁺ ions to the fluences from 10¹² to 10¹⁴ cm⁻² and the effects of irradiation were studied using ERDA, RBS and FTIR methods. The irradiation leads to release of hydrogen from the PEEK surface layer modified by the ion beam. The release is mild for low ion fluences but it becomes more pronounced at the ion fluences above 10¹³ cm⁻². At highest ion fluences the hydrogen concentration falls to 20-35% of its initial value. In contrast to hydrogen no significant oxygen release was observed. The kinetic of the hydrogen release is similar for the three ion species. FTIR measurement shows deep structural changes of the polymer structure resulting from the ion irradiation.     

Swift heavy ion induced structural modifications in zircon and scheelite phases of ThGeO4

Structural modifications in the zircon and scheelite phases of ThGeO₄ induced by swift heavy ions (93 MeV Ni⁷⁺) at different fluences as well as pressure quenching effects are reported. X-ray diffraction and Raman measurements at room temperature on the irradiated zircon phase of ThGeO₄ indicate the occurrence of stresses that lead to a reduction of the cell volume up to 2% followed by its transformation to a mixture of nano-crystalline and amorphous scheelite phases. Irradiation of the zircon phase at liquid nitrogen temperature induces amorphization at a lower fluence (7.5 × 10¹⁶ ions/m²), as compared to that at room temperature (6 × 10¹⁷ ions/m²). Scheelite type ThGeO₄ irradiated at room temperature undergoes complete amorphization at a lower fluence of 7.5 × 10¹⁶ ions/m² without any volume reduction. The track radii deduced from X-ray diffraction measurements on room temperature irradiated zircon, scheelite and low temperature irradiated zircon phases of ThGeO₄ are, 3.9, 3.5 and 4.5 nm, respectively. X-ray structural investigations on the zircon phase of ThGeO₄ recovered after pressurization to about 3.5 and 9 GPa at ambient temperature show the coexistence of zircon and disordered scheelite phases with a larger fraction of scheelite phase occurring at 9 GPa. On the other hand, the scheelite phase quenched from 9 GPa shows crystalline scheelite phase pattern.     

Ion irradiation damage effects in δ-phase Y6W1O12

Polycrystalline Y₆W₁O₁₂ samples were irradiated with 280 keV Kr²⁺ ions to fluences up to 2 × 10²⁰ ions/m² at cryogenic temperature (100 K). Ion irradiation damage effects in these samples were examined using grazing incidence X-ray diffraction (GIXRD) and cross-sectional transmission electron microscopy (TEM). The pristine Y₆W₁O₁₂ possesses rhombohedral symmetry (structure known as the δ-phase), which is closely related to cubic fluorite structure. GIXRD and TEM observations revealed that the irradiated Y₆W₁O₁₂ experiences an ordered rhombohedral to disordered cubic fluorite transformation by a displacement damage dose of ∼12 displacements per atom (dpa). At the highest experimental dose of ∼50 dpa, the uppermost irradiated region was found to be partially amorphous while the buried damage region was found to contain the same fluorite structure as observed at lower dose.     

Structural and optical study of irradiation effect in GaN epilayers induced by 308 MeV Xe ions

Wurtzite GaN epilayers irradiated at room temperature with 308 MeV ¹²⁹Xe³⁵⁺ ions to fluences of 1 × 10¹³ and 3 × 10¹³ cm⁻² have been studied by contact mode atomic force microscopy (AFM), high-resolution X-ray diffraction (HRXRD), micro-Raman scattering and photoluminescence (PL) spectroscopy. The AFM images showed that the surface of GaN films was etched efficiently due to the Xe ion irradiation. The initial step-terrace structure on GaN surface was eliminated completely at a fluence of 3 × 10¹³ cm⁻². HRXRD and Raman results indicated that the Xe ion irradiation led to a homogenous lattice expansion throughout the entire ∼3 μm-thick GaN films. The lattice expansion as well as the biaxial compressive stress of the films was increasing with the increase of ion fluence. PL measurements showed that a dominant yellow luminescence band in the as-grown GaN films disappeared, but a blue and a green luminescence bands were produced after irradiation. Based on these results, the strong electronic excitation effect of 308 MeV Xe ions in GaN is discussed.     

Anisotropic deformation of polystyrene particles by MeV Au ion irradiation

MeV Au irradiation leads to a shape change of polystyrene (PS) and SiO₂ particles from spherical to ellipsoidal, with an aspect ratio that can be precisely controlled by the ion fluence. Sub-micrometer PS and SiO₂ particles were deposited on copper substrates and irradiated with Au ions at 230 K, using an ion energy and fluence ranging from 2 to 10 MeV and 1 × 10¹⁴ ions/cm² to 1 × 10¹⁵ ions/cm². The mechanisms of anisotropic deformation of PS and SiO₂ particles are different because of their distinct physical and chemical properties. At the start of irradiation, the volume of PS particles decrease, then the aspect ratio increases with fluence, whereas for SiO₂ particles the volume remains constant.     

Structural, thermal and optical behavior of 84 MeV oxygen and 120 MeV silicon ions irradiated PES

In order to study structural, thermal and optical behavior, thin flat samples of polyethersulfone were irradiated with oxygen and silicon ions. The changes in properties were analyzed using different techniques viz: X-ray diffraction, thermo-gravimetric analysis, Fourier transform infrared, UV-visible and photoluminescence spectroscopy. A noticeable increase in the intensity of X-ray diffraction peaks was observed after irradiation with 84 MeV oxygen ions at low and medium fluences, which may be attributed to radiation-induced cross-linking in polymer. Fourier transform infrared and thermo-gravimetric analysis corroborated the results of X-ray diffraction analysis. No noticeable change in the Fourier transform infrared spectra of oxygen ion irradiated polyethersulfone were observed even at the highest fluence of 1 × 10¹³ ions cm⁻², but after irradiation with silicon ions, a reduction in intensity of almost all characteristic bands was revealed. An increase in the activation energy of decomposition of polyethersulfone was observed after irradiation with 84 MeV oxygen ions up to medium fluences but degradation was revealed at higher fluences. Similar trends were observed by photoluminescence analysis.