Spectral analysis method for deriving RBS-like carbon spectra from the C(α,α)C resonant reaction

This article presents a spectral analysis method that detects C using the high-sensitivity of the 4.26 MeV resonance of the ¹²C(α,α)¹²C nuclear reaction while avoiding issues arising from the peaky and asymmetric resonance shape, which complicates depth-sensitive C analysis. By averaging nuclear reaction spectra taken with a set of conveniently chosen He beam energies, we obtain C spectra with amplified intensity, but shape similar to Rutherford backscattering spectrometry (RBS) spectra. The latter fact allows intuitive reading of underlying C depth profiles without employing spectrum simulation software. The method was first applied to simulated samples whose nuclear reaction spectra were generated by SIMNRA, which allowed checking for method accuracy by comparison to corresponding simulated RBS spectra. As real examples of the method application, it was applied to detect depth-sensitive C signals from SiC substrates covered by SiO₂ layers and from 50 nm hafnium-based films deposited on Si by metal-organic chemical vapor deposition.     

Calculation and analysis of proton-induced reactions on Ni at incident energies from threshold to 200 MeV

Proton-induced reactions on ⁵⁸Ni have been studied in the energy range from threshold to 200 MeV. Based on experimental data of elastic scattering angular distributions and nonelastic cross section, an optimal set of proton optical potential parameters for ⁵⁸Ni has been obtained. All cross sections, elastic and inelastic scattering angular distributions, energy spectra and especially double differential cross sections for neutrons, protons, deuterons, tritons, helium particles and alpha particles emission have been calculated, using nuclear models theory. Theoretical calculations have been compared with existing experimental data, in most cases, the calculated results are in good agreement with the experimental data.     

A thin-layer reference material for hydrogen analysis

In many areas of material sciences, hydrogen analysis is of particular importance. For example, hydrogen is most abundant as impurity in thin film materials - depending on the deposition process - and has great influence on the chemical, physical and electrical properties of many materials. Existing bulk reference materials (RMs) are not suited for surface sensitive analytical methods like elastic recoil detection analysis (ERDA) or nuclear reaction analysis (NRA). To overcome this serious lack of (certified) thin-layer reference materials for the determination of hydrogen in the near-surface region (1-2 μm depth), we produced stable, homogeneous amorphous silicon layers on Si-wafers (aSi:H-Si) by means of chemical vapour deposition (CVD), while about 10% of hydrogen was incorporated in the Si-layer. Homogeneity and stability were proved by NRA whereas traceability of reference values has been assured by an international interlaboratory comparison.     

Measurement of neutron total cross-section and resonance parameters of xenon

We measured the neutron total cross-sections of natural xenon in the neutron energy region from 0.1 to 40 eV by using the time-of-flight method at the Pohang neutron facility, which consists of an electron linear accelerator, a water-cooled tantalum target with a water moderator, and a 12-m long time-of-flight path. A ⁶Li-ZnS(Ag) scintillator with a diameter of 12.5 cm and a thickness of 1.6 cm was used as a neutron detector. Notch filters composed of Co, In, Cd were used to estimate the background level and to calculate the neutron flight path length. The present measurement was compared with the existing experimental and the evaluated data. The resonance parameters of Xe isotopes were obtained from the transmission ratio by using the SAMMY code and were compared with other previous results.     

The total cross section and resonance parameters for the 0.178 eV resonance of Cd

It has been suggested that the capture and scattering cross sections of natural cadmium are not well described by the resonance parameters that are given in the evaluated data files. In particular, doubts on the parameters of the first resonance of ¹¹³Cd at 0.178 eV have been raised. This resonance is of high importance in the interpretation in many integral experiments, such as neutron activation analysis, in which cadmium foils are used to shield from thermal neutrons. A new set of experiments has been designed and performed at the neutron time-of-flight facility GELINA, to determine the total cross section and to extract a set of resonance parameters. The covariance information of the experimental data is propagated and the correlation between the resonance parameters is derived. The obtained parameters are then compared to the data available in the literature. Finally a set of criticality experiments from the international handbook of evaluated critical safety benchmark experiments is used to quantify the influence of the change in the resonance parameters.     

Deuterium inventory in plasma facing materials by means of NRA: A microbeam probe approach

Particle retention in tokamak walls is a key issue for long time discharges in future thermonuclear fusion reactors. Plasma wall interactions drive the fuel retention through two major mechanisms: co-deposition with carbon produced by wall erosion and particle retention in wall materials. In this study, we report results obtained from the tokamak Tore Supra, from which two types of samples were analyzed by means of micro-NRA: (i) small pieces of deposited carbon layers were collected after cumulative discharges and deuterium contents were measured; (ii) carbon fiber composite (CFC) samples, immersed in the plasma during an experimental campaign were also analyzed. 3D deuterium elemental mapping demonstrated that deuterium can be trapped at depths much higher than usual implantation depths and deep local retention sites have been evidenced and localized.This study demonstrates that μNRA can be used for assessment of deuterium post-mortem inventory in tokamaks, both by measuring uniformly distributed deuterium in small fragments of deposited carbon layers and by locally describing deuterium 2D and 3D distributions in complex structures.     

Calculation and evaluation of cross-sections for p+Fe reactions up to 250 MeV

All cross-sections of proton-induced reactions, angular distributions and the energy spectra of neutron, proton, deuteron, triton, helium and alpha-particle emission are consistent calculated and analyzed for p+^{54,56,57,58,nat}Fe at incident proton energies below 250 MeV by using nuclear theoretical models which integrate the optical model, the intra-nuclear cascade model, direct, preequilibrium and equilibrium reaction theories. Especially, the cross-sections of the light composite particle (d, t, ³He and α) emissions are improved based on the exciton model including the pick-up mechanism. Theoretical calculated results are compared with existing experimental data.     

Scanning-PIXE analysis of gold lace embroideries in a relic of St. Francis

In this work, we describe the compositional analysis performed by scanning-mode PIXE on the metal threads of a XIII century embroidery. The precious work analysed is the pillow-case used to cover the pillow, on which - according to tradition - St. Francis of Assisi was resting his head when he died. Measurements were performed in order to characterise the embroideries of the two sides and the passementerie in the lateral hems. Several areas, each of the order of two square millimetres, were scanned with a 3 MeV proton external beam of 20 μm size on target, using the external micro-beam facility of our laboratory, with list-mode acquisition. Analysis of elemental maps and spectra from selected homogeneous sub-areas allowed us to extract the quantitative composition of the gilded tape and estimates of its thickness.     

Study of the useful yield of the Storing Matter technique using Ge(1 0 0) as a sputter target

Storing Matter is a new analytical technique for organic and inorganic materials, which tries to circumvent the well-known matrix effect in SIMS. This technique consists of separating the sputtering of the sample from the subsequent analysis steps. Thus, the sample to be analysed is sputtered with a focused ion beam produced by a floating low-energy ion gun (FLIG) and the particles emitted under the ion impacts are deposited at a sub-monolayer level on a well-known collector. The collector with the deposited material is then analysed in a second step by SIMS (dynamic and static mode). The main advantage of this new technique is to improve the sensitivity and the quantification of the SIMS analysis. All the processes, including all the sample and collector transfers, are performed in UHV conditions. This paper presents preliminary results obtained on the Storing Matter prototype instrument developed in our laboratory. The sputtering of a (1 0 0) Ge wafer by ions was used as a model system to study the influence of using different collector surfaces (W, Ta and Al) on the Storing Matter useful yield.     

Determining Pu isotopic composition and Pu content of PuBe sources by neutron coincidence technique

The paper describes a pure neutron method for determining both Pu content and Pu isotopic composition of PuBe neutron sources by neutron coincidence technique, without using gamma-spectrometry. The new procedure based on the R/T-T relationship is a developed version of the R/T-method based on R/T-M_Pu calibration curve described in [C.T. Nguyen, J. Bagi, L. Lakosi, A novel method of quantitative assay of PuBe neutron sources by neutron coincidence technique, Nucl. Instr. and Meth. B 246 (2006) 409], utilizing Pu isotopic correlations; here R, T, M_Pu are double count rate, single count rate and total Pu content, respectively. Accuracy of the method was found to be about 2-3% and 15% for ²³⁹Pu component and Pu content, respectively. Measurement time as a function of detector efficiency is treated in detail. It is shown that in a system of frame, a transuranium neutron source can be characterized by a pair of co-ordinates [R/T,  T].     

Light charged particle emission for p+Fe reactions

The energy spectra and double differential cross sections of nucleon and the light composite particle (d, t, ³He and α) emissions are studied based on the exciton model included the improved Iwamoto-Harada model. All cross sections of proton induced reactions, angular distributions and energy spectra are consistent calculated and analyzed for ^{54,56,57,58,nat}Fe at incident proton energies below 250 MeV by using nuclear theoretical models which integrate the optical model, the intra-nuclear cascade model, direct, pre-equilibrium and equilibrium reaction theories. Theoretical calculated results are compared with existing experimental data.     

Evaluation of neutron cross sections for a complete set of Dy isotopes

Neutron cross sections for a complete set of Dy isotopes, ^{156,158,160,161,162,163,164}Dy, were evaluated in the incident energy range from 10⁻⁵ eV to 20 MeV. In the low energy region, including thermal and resolved resonances, our evaluations are based on the latest data published in the Atlas of Neutron Resonances. In the unresolved resonance region we performed additional evaluation by using the averages of the resolved resonances and adjusting them to the experimental data. In the fast neutron region, we used the nuclear reaction model code EMPIRE-2.19 with the model parameters adjusted to the experimental data. The results are compared with the available experimental data and with the existing nuclear data libraries, including ENDF/B-VI.8 and JEFF-3.1. The new evaluations are suitable for neutron transport calculations and they were adopted by the new US evaluated nuclear data library, ENDF/B-VII.0, released in December 2006.     

Cross sections for the production of helium, neon and argon isotopes by proton-induced reactions on iron and nickel

We measured integral thin target cross sections for the proton-induced production of ³He, ⁴He, ²¹Ne, ²²Ne, ³⁶Ar and ³⁸Ar from Fe and Ni from the respective reaction thresholds up to 1.6 GeV. The production of noble gas isotopes, especially ⁴He, from Fe and Ni is of special importance for design studies of accelerator driven systems and/or energy amplifier, because Fe is the main structural material in almost every design study. Furthermore, the cross sections are needed to establish the first physical model calculations for the production of cosmogenic nuclides in iron meteorites. As a result of our new measurements there now exist for both target elements a complete and consistent database for the production of noble gas isotopes. The experimental data are compared to results from the theoretical nuclear model codes INCL4/ABLA and TALYS. This comparison clearly demonstrates again that experimental data are still needed because the predictive power of nuclear model codes, though permanently improving, does still not allow reliably predicting the cross sections needed for most applications and irradiation experiments remain indispensable.     

Differential and scanning-mode external PIXE for the analysis of the painting “Ritratto Trivulzio” by Antonello da Messina

Extensive PIXE investigations have been performed at the LABEC accelerator laboratory in Florence on the painting “Ritratto Trivulzio” by Antonello da Messina, one of the great Italian masters of XV Century and a pioneer in modern oil painting.It is well known that a complete and unambiguous characterisation of materials in paintings is often difficult, owing to their complex structure. For the “Ritratto Trivulzio”, the combination of advanced variants of PIXE, such as differential and scanning-mode analysis, provided a relevant contribution to the characterisation of paint layers, in terms of composition and structure, in a totally non-invasive and non-destructive way.Single-spot mode PIXE with external proton beams of about half millimetre diameter was first used for a general characterisation of different areas of the painting. Differential PIXE performed in many spots led to reconstruct the sequence of paints employed by the artist and to estimate in some cases the local paint layer thickness.A second run carried out with the external scanning microbeam facility, using a 3 MeV proton beam of about 80 μm size, was then crucial to clarify some issues raised by the first analysis. In particular, elemental maps from selected areas helped to understand the way some colour shades had been obtained on the red mantle of the portrayed gentleman, using different pigments irregularly distributed on the surface.     

Heat deposition in thick targets due to interaction of high energy protons and thermal hydraulics analysis

Heat deposition inside thick targets due to interaction of high energy protons (E_p ∼ GeV) has been estimated using an improved version of the Monte Carlo simulation code CASCADE.04.h. The results are compared with the available experimental data for thick targets of Be, Al, Fe, Cu, Pb and Bi at proton energies of 0.8 GeV, 1.0 GeV and 1.2 GeV. A more continuous heat deposition approach which has been adopted in CASCADE.04.h yields results which are in better agreement with the experimental data as compared to the ones from the earlier version of CASCADE.04. The results are also compared with the predictions of the FLUKA Monte Carlo code. Both CASCADE.04.h and FLUKA predictions are nearly similar for heavy targets and both agree with the experimental measurements. However, they do have differences in predictions for lighter targets where measurements also differ from the predictions. It is observed that the maximum heat loss in thick targets occurs at the beginning of the target due to increasing nuclear reaction contributions. This aspect is crucial in designing the window of a spallation neutron target employed in an accelerator driven sub-critical system (ADS) as this is the first material to be traversed by the proton beam and is subjected to the maximum temperature gradient. Optimization of the target-window parameters requires a careful estimation of heat deposition in the window region and this has been demonstrated through thermal hydraulic studies related to the design of a realistic lead bismuth eutectic (LBE) spallation neutron target for an ADS system.     

Investigation of the Zn(p, 2p)Cu nuclear reaction: New measurements up to 40 MeV and compilation up to 100 MeV

The excitation function was measured for the ⁶⁸Zn(p, 2p)⁶⁷Cu nuclear reaction from its threshold energy up to 40 MeV. Nine pieces of highly enriched ⁶⁸Zn (>98%) metal foils were irradiated to obtain reliable cross-sections using the usual stacked-foil technique. All foils were subjected to high efficiency radiochemical separation before the activity measurements. A critical compilation of the available experimental cross-section results was also performed. Thick target yields of ⁶⁷Cu and the longer-lived copper radio-contaminants (⁶¹Cu and ⁶⁴Cu) were calculated using the reliable literature results up to 100 MeV. Additionally, EOB (End Of Bombardment) contamination levels as a function of bombarding energy and irradiation time were deduced.     

Production of noble gas isotopes by proton-induced reactions on bismuth

We measured integral thin target cross sections for the proton-induced production of He-, Ne-, Ar-, Kr- and Xe-isotopes from bismuth (Bi) from the respective reaction thresholds up to 2.6 GeV. Here we present 275 cross sections for 23 nuclear reactions. The production of noble gas isotopes from Bi is of special importance for design studies of accelerator driven systems (EA/ADS) and nuclear spallation sources. For experiments with proton energies above 200 MeV the mini-stack approach was used instead of the stacked-foil technique in order to minimise the influences of secondary particles on the residual nuclide production. Comparing the cross sections for Bi to the data published recently for Pb indicates that for ⁴He the cross sections for Bi below 200 MeV are up to a factor of 2-3 higher than the Pb data, which can be explained by the production of α-decaying Po-isotopes from Bi but not from Pb. Some of the cross sections for the production of ²¹Ne from Bi are affected by recoil effects from neighboured Al-foils, which compromises a study of a possible lowering of the effective Coulomb-barrier. The differences in the excitation functions between Pb and Bi for Kr- and Xe-isotopes can be explained by energy-dependent higher fission cross sections for Bi compared to Pb. The experimental data are compared to results from the theoretical nuclear model codes INCL4/ABLA and TALYS. The INCL4/ABLA system describes the cross sections for the production of ⁴He-, Kr- and Xe-isotopes reasonably well, i.e. mostly within a factor of a few. In contrast, the model completely fails describing ²¹Ne, ²²Ne, ³⁶Ar and ³⁸Ar, which are produced via spallation and/or multifragmentation. The TALYS code is only able to accurately predict reaction thresholds. The absolute values are either significantly over- or underestimated. Consequently, the comparison of measured and modelled thin target cross sections clearly indicates that experimental data are still needed because the predictive power of nuclear model codes, though permanently improving, does still not allow to reliably predict the cross sections needed for most applications and irradiation experiments remain indispensable.     

PIXE measurements of Renaissance silverpoint drawings at VERA

Silverpoint drawings from the Renaissance are among the most precious and rarest treasures of graphical art. Our research group is particularly interested in the analysis of silverpoint drawings by Albrecht Dürer (1471-1528). A very sensitive and non-destructive analytical method, either spatially resolved synchrotron-radiation induced X-ray fluorescence (SY-XRF) or proton-induced X-ray emission (PIXE), is needed to determine the chemical composition of the very faint silver marks on such drawings. Dürer drawings from the collection of the Albertina, Vienna, were analyzed to amend existing data on Dürer drawings. For this purpose an external-beam PIXE setup was installed at the Vienna Environmental Research Accelerator (VERA). It allows to analyze a spot of ∼0.15 mm on the object in air with 3 MeV protons, and to detect the emitted X-rays that are characteristic for the chemical composition with very good sensitivity and without harming the precious objects. After successful measurements on artificial test samples, four original silverpoint drawings were investigated: two portraits from Albrecht Dürer’s very early period (self-portrait and portrait of his father) and two drawings from Dürer’s sketch book of his travel to the Netherlands 1520/21.     

PIXE as a complement to trace metal analysis of sediments by ICP-OES

The adverse effects of metal contamination in sediments require methods that can quickly and accurately assess the extent of environmental pollution. Particle induced X-ray emission spectrometry (PIXE) is demonstrated to be a viable alternative to an established method, which consists of acid digestion and Inductively coupled plasma-optical emission spectrometry (ICP-OES) to measure trace metals in sediment. The analysis of trace metal composition by both techniques on a NIST Standard Reference Material mud gives results that are consistent with the certified values for fourteen measured metals, seven of which are common to both methods. A comparison study conducted on a sediment core from a freshwater lake with a known chromium contamination in Muskegon County, MI also shows a good correlation between the methods for transition metals of environmental interest over a wide range of metal concentrations. Total sample preparation and analysis time for the PIXE measurements is roughly one third that of acid digestion and ICP-OES. Also, the acid digestion step does not elute all the metal, while the nondestructive PIXE approach is a total metals analysis method. However the PIXE method generally has higher limits of detection for many environmental metal contaminants. By combining the two techniques, the acid digestion elution factor can be quantified by running PIXE on an original sample and on the residue resulting from acid digestion.     

Characteristics comparison between a cyclotron-based neutron source and KUR-HWNIF for boron neutron capture therapy

At Kyoto University Research Reactor Institute (KURRI), 275 clinical trials of boron neutron capture therapy (BNCT) have been performed as of March 2006, and the effectiveness of BNCT has been revealed. In order to further develop BNCT, it is desirable to supply accelerator-based epithermal-neutron sources that can be installed near the hospital. We proposed the method of filtering and moderating fast neutrons, which are emitted from the reaction between a beryllium target and 30-MeV protons accelerated by a cyclotron accelerator, using an optimum moderator system composed of iron, lead, aluminum and calcium fluoride. At present, an epithermal-neutron source is under construction from June 2008. This system consists of a cyclotron accelerator, beam transport system, neutron-yielding target, filter, moderator and irradiation bed.In this article, an overview of this system and the properties of the treatment neutron beam optimized by the MCNPX Monte Carlo neutron transport code are presented. The distribution of biological effect weighted dose in a head phantom compared with that of Kyoto University Research Reactor (KUR) is shown. It is confirmed that for the accelerator, the biological effect weighted dose for a deeply situated tumor in the phantom is 18% larger than that for KUR, when the limit dose of the normal brain is 10 Gy-eq. The therapeutic time of the cyclotron-based neutron sources are nearly one-quarter of that of KUR. The cyclotron-based epithermal-neutron source is a promising alternative to reactor-based neutron sources for treatments by BNCT.