Differential cross-section measurements for the C(d, p0)C reaction and applications to surface analysis of materials

This work involves surface analysis by nuclear techniques, which are non-destructive, and computer simulation. The “energy analysis” method for nuclear reaction analysis is used. Energy spectra are computer simulated and compared to experimental data, giving target composition and concentration profile information. Measured values are presented for the differential cross-section of the ¹²C(d, p₀)¹³C reaction in the deuteron energy range 0.81-2.07 MeV for laboratory detection angles of 165° and 135°, using self-supported two-layered targets consisting of high purity thin films of typically 13 μg/cm² natural carbon and 65 μg/cm² gold. The error in the absolute differential cross-section values is generally ∼6%. The method, using these values, is successfully applied to determination of uniform concentration profiles of ¹²C, along considerable depths, for a thick flat target of high purity pyrolitic graphite. It is characterised a thin surface film of carbon on a thick flat quartz target. Uniform concentration profiles of ¹⁶O are also obtained from (d, p) and (d, α) reactions.     

Tritium Depth Profiling Study on Titanium Tritide Target for Generating 14-MeV Neutrons

In-situ measurements of the depth profiles of tritium in a titanium tritide target for generating 14-MeV neutrons have been made with the method of the ion beam analysis using the T(d, α)n nuclear reaction. The initial distribution of tritium in the unirradiated target has been observed to be nearly uniform over the depths. After the irradiation of 390-keV D₃ ⁺ ions at a temperature of about 10°C a dip has been found in the depth profile around the depth of the projected range of the ions. By the successive isochronal anneal-ings at temperatures below 130°C the tritium has been uniformly redistributed. The behavior of tritium in the target and the effectiveness of the depth profiling for evaluating the energy spectrum and the yield of source neutrons are discussed.     

RNRA and neutron threshold analyses of thick lithium coatings deposited by sputter evaporation

Li coatings on various substrates have numerous applications: Boron neutron capture therapy, super conducting tokamak, etc.Unfortunately the main difficulty using Li is its reactivity in air and diffusion into metals. It is the only metal that reacts with nitrogen at room temperature and it tarnishes and oxidizes rapidly in air.In this work, we investigate how to profile thick Li layers (50 μm) deposited on SiO₂ substrates by a method based on plasma sputtering, involving both DC sputtering and evaporation simultaneously.A thick Li layer (≈10 μm) was covered with a thin stainless steel layer to prevent oxidation during transfer of the sample from the sputtering chamber and the accelerator. Li coatings were investigated by RNRA and neutron threshold reaction to obtain interdiffusion profiles of the different components and their concentration. The depth profile using the ⁷Li(p,γ)⁸Be^∗ resonance nuclear reaction occurring at 440 keV allows us to obtain Li concentration versus depth up to 50 μm.Preliminary results indicate that homogeneous Li layers can be obtained and protected against air, even though it diffuses into the encapsulated layers.     

Determination of the concentrations of tritium and helium in titanium tritide targets

Atom ratios of T to Ti in T-Ti targets have been determined by the ⁴He⁺ Rutherford backscattering (RBS) and the proton elastic scattering (PES) techniques, and that of ³He to T in aged T-Ti targets by the ³He(d, p)⁴He and T(d, n)⁴He reactions. The results from RBS show that the depth distribution of T is uniform in a region of 8000 Å under the target surface. For the results from the nuclear reaction analysis (NRA), a discrepancy between the experimentally measured and the calculated concentration of ³He in a heavily bombarded T-Ti target obviously exists.     

Nuclear reactions induced by deuterons and their applicability to skin tumor treatment through BNCT

In this work the D(d,n)³He and ⁹Be(d,n)¹⁰B reactions have been studied in a low-energy regime as neutron sources for skin tumor treatment in the frame of accelerator-based BNCT (AB-BNCT). The total neutron production and the energy and angular distributions for each reaction at different bombarding energies and for the thick targets considered (TiD₂, Be) have been determined using the available data in the literature. From this information, a feasibility study has been performed by means of MCNP simulations. The thermal, epithermal and fast neutron fluxes and doses at skin tumor positions (loaded with 40 ppm ¹⁰B) which are located on a whole-body human phantom have been simulated for different D₂O moderator depths. The best-case performance shows that a high tumor control probability (TCP) of 99% corresponding to a weighted dose in tumor of 40 Gy can be reached at the tumor position keeping the weighted dose in healthy tissue below 12.5 Gy, by means of the ⁹Be(d,n)¹⁰B reaction at 1.1 MeV for a deuteron current of 20 mA and a 30 cm D₂O moderator in 52 min. The availability of low-energy neutrons in the ⁹Be(d,n)¹⁰B reaction from the population of excited levels between 5.1 to 5.2 MeV in ¹⁰B and the convenience of a thin beryllium target are discussed.As a complement concerning alternatives to the Li(metal) + p reaction, the neutron yield of refractory lithium compounds (LiH, Li₃N and Li₂O) were calculated and compared with a Li metal target.     

A simple coincidence method of deuterium profiling using the DHe, α)H reaction

A simple standard coincidence arrangement is described for D(³He, α)H depth profiling experiments of deuterium in solids. Both reaction products are detected in coincidence, the high-energy protons being observed in transmission through a foil target. The energy of the α-particles is converted into the corresponding depth scale, whereas the local deuterium concentration is calculated from the yield of the α-particle spectrum. The measurement of α-particles in coincidence with protons allows a reduction of background arising from Rutherford scattering of ³He and other reaction products. For samples of deuterium implanted into Ta₂O₅ and Er, the method allows a reduction of the backscattering yield by a factor of more than 10³. The residual background is due to accidental coincidences. It can be even more reduced using an accurate experimental geometry. The background reduction is largest for samples with a low content of deuterium, allowing measurements of deuterium profiles of 9 × 10¹³ D⁺/cm² implanted into Ta₂O₅ at an energy of 8 keV. This corresponds to a maximum deuterium concentration of about 5 × 10⁻⁴ D per Ta₂O₅. This method is not restricted to thin films, but it allows measurements of deuterium profiles in a thick sample, e.g. of an implantation profile in a 0.4 mm silicon wafer.     

Depth distribution profiling of deuterium and 3He

A technique using nuclear microanalysis has been developed to determine ²D an ³He concentrations versus depth profiles in the near surface regions (～2 μm) of solids. Ultimate near-surface depth resolutions of (≈100 Å) should be attainable by these techniques. A probing beam of ³He ions is used to analyze for the deuterium. By energy analyzing the emitted ⁴He ions from the reaction d(³He,p)⁴He and by simple computer analysis, deuterium concentration versus depth profiles are obtained. The same methods are applicable for ³He profiling except in that case a ²D probing beam is used. The techniques is currently being developed using Er hydride and Sc hydride films. It is particularly suited for the study of the transition metals with high hydrogen solubility such as Nb and V which are of interest for CTR reactor applications.     

Depth profiling of Mg by 2010 keV resonance of Mg(p,p′γ)Mg nuclear reaction

Studies on the characteristics of 2010 keV resonance in ²⁴Mg(p,p′γ)²⁴Mg nuclear reaction for depth profiling Mg in thin films are reported. The resonance reaction, based on the detection of characteristic 1368 keV γ-rays, enables interference free measurement of Mg down to 2 × 10²⁰ atoms/cm³ and has a probing depth of about 20 μm. The width of the resonance extracted from excitation curves for thick (>180 nm) thermally grown elemental Mg films, by SPACES is about 350 ± 50 eV. The reaction has been used to depth profile Mg in a Mg/Ti/Mg/Si film which provides interesting information on interfacial mixing involving Ti layer and the underlying Mg layer.     

Measurement of differential cross-sections and widths of resonances in S(p,p′γ) S reaction in the 3.0-4.0 MeV region

The paper reports the widths and differential cross-sections of resonances at 3.089, 3.379 and 3.717 MeV in the ³²S(p,p′γ)³²S nuclear reaction. The cross-sections are computed at 0° and 90° angles (relative to the beam direction) from thick target excitation curves constructed by measuring 2230 keV γ-rays, characteristic of the reaction. The differential cross-sections of resonances are about 18, 64 and 70 mb/sr respectively at 0° angle and decrease by about half around an angle of 90°. The first resonance, the sharpest among the three, exhibits a width of about 400 eV while those at 3.379 and 3.717 MeV are in 1.0-1.5 keV range. The widths of the resonances are extracted from the respective thick target excitation curves by an interquartile separation method and also by simulating their leading edges. A study of thick target yields in the 3.0-4.0 MeV proton energy region for several sulphide forming elements shows the absence of any significant interference. These resonances, as a result, can be effectively utilised for sensitive and high resolution depth profile measurements of sulphur in films and materials surfaces.     

PIGE analysis and profiling of aluminium

In this work we present an alternative method for PIGE analysis of aluminium in thick samples. This method is based on the ERYA - emitted radiation yield analysis - code, which integrates the nuclear reaction excitation function along the depth of the sample. For this purpose, the excitations functions of the ²⁷Al(p,p′γ_1,2)²⁷Al reaction (with gamma-ray energies of 844 and 1014 keV) were employed. Calculated gamma-ray yields were compared, at several proton energy values, with experimental yields for thick samples made of inorganic compounds containing aluminium. The agreement is better than 5%.The 1684 keV resonance of the same reaction, with a natural width of 100 eV, was used to profile samples of Ti implanted with several doses of Al. We show that this resonance, stronger than the 992 keV resonance of the ²⁷Al(p,γ)²⁸Si usually employed for aluminium profiling, leads to similar depth resolution in shorter collection time.     

Method to measure composition modifications in polyethylene terephthalate during ion beam irradiation

Matter losses of polyethylene terephthalate (PET, Mylar) films induced by 1600 keV deuteron beams have been investigated in situ simultaneously by nuclear reaction analysis (NRA), deuteron forward elastic scattering (DFES) and hydrogen elastic recoil detection (HERD) in the fluence range from 1 × 10¹⁴ to 9 × 10¹⁶ cm⁻². Volatile degradation products escape from the polymeric film, mostly as hydrogen-, oxygen- and carbon-containing molecules. Appropriate experimental conditions for observing the composition and thickness changes during irradiation are determined. ¹⁶O(d,p₀)¹⁷O, ¹⁶O(d,p₁)¹⁷O and ¹²C(d,p₀)¹³C nuclear reactions were used to monitor the oxygen and carbon content as a function of deuteron fluence. Hydrogen release was determined simultaneously by H(d,d)H DFES and H(d,H)d HERD. Comparisons between NRA, DFES and HERD measurements show that the polymer carbonizes at high fluences because most of the oxygen and hydrogen depletion has already occured below a fluence of 3 × 10¹⁶ cm⁻². Release curves for each element are determined. Experimental results are consistent with the bulk molecular recombination (BMR) model.     

Generalized analysis method for neutron resonance transmission analysis

Neutron resonance densitometry (NRD) is a non-destructive analysis method, which can be applied to quantify special nuclear materials (SNM) in small particle-like debris of melted fuel that are formed in severe accidents of nuclear reactors such as the Fukushima Daiichi nuclear power plants. NRD uses neutron resonance transmission analysis (NRTA) to quantify SNM and neutron resonance capture analysis (NRCA) to identify matrix materials and impurities. To apply NRD for the characterization of arbitrary-shaped thick materials, a generalized method for the analysis of NRTA data has been developed. The method has been applied on data resulting from transmission through thick samples with an irregular shape and an areal density of SNM up to 0.253 at/b (≈100 g/cm²). The investigation shows that NRD can be used to quantify SNM with a high accuracy not only in inhomogeneous samples made of particle-like debris but also in samples made of large rocks with an irregular shape by applying the generalized analysis method for NRTA.     

Determination of deuterium in dead-sea water by nuclear methods

By using the D(d, p)³H nuclear reaction combined with the Rutherford-backscattering method, the amount of D₂O in relation to H₂O in water from the Dead Sea is measured. The amount of deuterium in the samples is determined from the integrated yield of the D(d, p)³H reaction in relation to the ¹⁶O(d, p₀)¹⁷O or ¹⁶O(d, p₁)¹⁷O reaction. For the low deuteron energies used (E 0.63 MeV), the differential cross section of the ¹⁶O(d, p₀)¹⁷O reaction was determined experimentally. No significant change of deuterium concentration in Dead-Sea water down to a depth of 36 m could be detected.     

Nanohardness and structure of nitrogen implanted SixAly coatings post-implanted with oxygen

“Sialons” have several interesting mechanical, thermal and chemical properties which make them candidates for high temperature applications. Solid solutions in the Si–Al–O–N system were synthesised using nitrogen and oxygen implantation into Si₃₃Al₆₇, Si₄₅Al₅₅ and Si₆₇Al₃₃ thin films deposited by DC magnetron sputtering on glassy carbon substrates. Nitrogen has been implanted firstly at 50 and then at 20 keV, oxygen was post-implanted at 50 keV. The different implantation doses ranged from 1 to 10 × 10¹⁷ ions/cm². High depth resolution profiles were obtained using RBS and resonant nuclear reaction, the chemical bonds were investigated using LEEIXS and these results are correlated to the film structure measured by cross section TEM. The TEM micrographs show a columnar structure perpendicular to the substrate surface in unimplanted coatings. Nevertheless, when nitrogen is implanted grain formation is observed and after oxygen post-implantation gas bubbles appear at the film depth where the maximum oxygen concentration is observed. The correlation of these results with RBS and LEEIXS measurements indicates that nitrogen should be enclosed in these bubbles. Nanohardness was also measured. The highest values are observed in samples post-implanted with 1 × 10¹⁷ O/cm² where nanohardness increases from 3 to 10 Gpa.     

Reduction of light elements loss in polymer foils during MeV-proton irradiation by application of an aluminum coating

Backscattering and forward-scattering spectrometry with 2.2 MeV-protons have been applied to detect light elements including H, C, N and O in polymer foils of aromatic polyimide (PI), polyethylene telephthalate (PET) and polyethylene naphthalate (PEN). In the case of PI, no significant loss of H, C, N and O was observed during proton irradiation. In the case of PET and PEN, on the other hand, all the light elements gradually decreased as irradiation fluence increased and the contents of 15%-H, 14%-C, 47%-O in PET and 7%-H, 5%-C 31%-O in PEN were eventually released up to a fluence of 2.1 × 10¹⁶ protons/cm². An aluminum thin film (thickness ∼0.1 μm) was sputter-deposited on the upper surface of 4 μm thick PET and PEN foils to prevent the release of light elements. In Al coated PEN foil, for example, the losses of H, C and O were 2%, 0.5% and 22% of the starting contents, respectively, considerably smaller than those found for uncoated PEN. Thus the Al coating was found to be an effective method to suppress the loss of constituent elements.     

Excitation functions of proton induced nuclear reactions on W up to 40 MeV

We measured the excitation functions for the production of the ^{181,182m,182g,183,184g,186}Re radioisotopes from proton bombardment of natural tungsten by using a stacked-foil activation technique in the energy range from threshold energy to 40 MeV at the MC50 cyclotron of the Korea Institute of Radiological and Medical Science. The results were compared with the earlier reported experimental data and the model calculations using codes TALYS and ALICE-IPPE. The present values are in good agreement with some of the previously reported literature. The integral yields for thick targets were also deduced from the measured excitation functions of the produced radioisotopes. The deduced yield values were compared with the available directly measured thick target yield, and found acceptable agreement. The investigated radioisotope ¹⁸⁶Re has remarkable applications in the field of nuclear medicine, whereas the data of ^183,184gRe have potential applications in thin layer activation analysis.     

A test of two depth profiling techniques using PIXE

A destructive and a nondestructive technique for depth profiling using PIXE is tested on various concentration profiles of Zn depletion in initially homogeneous Ag 3 at.% Zn alloys. The first consists of measuring the yield of X-rays emerging from thin film targets prepared by deposition of Ag and Zn hydroxides originating from slabs of controlled thickness removed from the analysed sample. The second consists of deconvoluting a set of X-ray yield measurements carried out with various energies. Both techniques are cross-referenced with electron microprobe analysis run on a transverse section of the corresponding specimens, but can also be applied to profiles extending over depths too small for analysis on a transverse section. Internal coherence between the different concentration profiles obtained is checked on the basis of Zn diffusivity in Ag-Zn alloys.     

Depth profiling of Al2O3 + TiO2 nanolaminates by means of a time-of-flight energy spectrometer

Atomic layer deposition (ALD) is currently a widespread method to grow conformal thin films with a sub-nm thickness control. By using ALD for nanolaminate oxides, it is possible to fine tune the electrical, optical and mechanical properties of thin films. In this study the elemental depth profiles and surface roughnesses were determined for Al₂O₃ + TiO₂ nanolaminates with nominal single-layer thicknesses of 1, 2, 5, 10 and 20 nm and total thickness between 40 nm and 60 nm. The depth profiles were measured by means of a time-of-flight elastic recoil detection analysis (ToF-ERDA) spectrometer recently installed at the University of Jyväskylä. In TOF-E measurements ⁶³Cu, ³⁵Cl, ¹²C and ⁴He ions with energies ranging from 0.5 to 10 MeV, were used and depth profiles of the whole nanolaminate film could be analyzed down to 5 nm individual layer thickness.     

Cross-section for D(p,p)D elastic scattering from 1.8 to 3.2 MeV at the laboratory angles of 155° and 165°

The D(p,p)D cross-sections for elastic scattering of proton on deuterium over incident proton energy range from 1.8 to 3.2 MeV at both laboratory angles of 155° and 165° were measured. A thin solid state target Ni/TiD_x/Ta/Al used for cross-section measurement was fabricated by firstly depositing layers of Ta, Ti and Ni film on the Al foil substrate of about 7 μm in turn using magnetron sputtering and then deuterating under the deuterium atmosphere. The areal density of metal element in each layer of film was measured with RBS analysis by using a 4.0 MeV ⁴He ion beam, while the areal density of the deuterium absorbed in the Ti film was measured with ERD analysis by using a 6.0 MeV ¹⁶O ion beam. The results show that the cross-sections of p-D scattering under this experimental circumstance were much enhanced over the Rutherford cross-section value. It was found that the enhancement increases linearly as the energy of the incident beam increases. The total uncertainty in the measurements was less than 7.5%.