Erratum to “Measurement of cross-sections for the (p, xn) reactions in natural molybdenum” [Nucl. Instr. and Meth. B 262 (2007) 171]

Using PIGE (TIARA, JAPAN) technique, we measured fluorine (F) uptake into the tooth enamel around a fluoride-containing material during caries progression using pH cycling. Class I cavities in the buccal surfaces of 6 extracted human teeth were drilled and filled with fluoride-containing material; a glass ionomer cement (Fuji IX(GC)). Three 300 μm sections through the material were obtained from each tooth. Two of these specimens were utilized to measure the F distribution in enamel adjacent to the material. A 1.7 MeV proton beam accelerated by the TIARA single-ended accelerator was delivered to a micro-beam apparatus. The beam spot size was about 1 μm with a beam current of about 100 pA. A nuclear reaction, ¹⁹F(p, αγ)¹⁶0, was used to measure the F concentration and the gamma-rays from this reaction were detected with a 4” NaI detector. X-rays induced by proton were detected with a Si(Li) detector to measure calcium concentration and the beam intensity was monitored with the X-ray yield from a copper foil for quantitative analysis. After measurement of F uptake, all specimens were polished to a thickness of 120 μm. In order to simulate daily acid challenges occurring in the oral cavity, the pH cycling (pH6.8–pH4.5) was carried out for 1, 3 and 5 weeks, separately. The duration that the solution remained below pH 5.5 was 37 min per cycle. The cycles were repeated 6 times per day with 2 h interval between cycles, and the specimens were kept in remineralizing solution for the rest of pH cycle. After pH cycling, F and calcium distribution of each specimen was evaluated using PIGE technique. The F distribution of the specimens before pH cycling clearly showed the F uptake from fluoride-containing material into enamel adjacent to the material. After pH cycling, the caries progression in all specimens was observed by the image of transverse microradiography (TMR). The depth of caries and mineral loss progressed with increasing the duration of pH cycling, although the enamel adjacent to the material remained a caries inhibition zone due to low rate of demineralization. With caries progression, fluorine accumulated in the subsurface of the caries lesion, while the outermost surface of the caries lesion gradually dissolved under increasing pH cycling. The data obtained using PIGE (TIARA, JAPAN) technique were useful to understand the fluorine benefit for preventing dental caries by means of fluoride-containing dental materials.     

Fluorine analysis of human enamel around fluoride-containing materials under different pH-cycling by μ-PIGE/PIXE system

The caries preventive effect of fluoride-containing materials (FCMs) might depend on the caries risk of the individuals. Two pairs of demineralizing and remineralizing solutions of pH-cycling were prepared for simulating low and high caries risk. The purpose of this study was to determine fluorine (F) uptake into human enamel around FCMs under different pH-cycling using the in-air μ-PIGE/PIXE system. Fluoride-containing glass ionomer cement (Fuji IX_GP FAST CAPSULE (FN)), and composite resin (BEAUTIFIL II with FLUORO BOND SHAKE ONE (BS)) were used in this study. The pH-cycling (pH 6.8-4.5) was carried out for 5 weeks. After pH-cycling, the caries progression was analyzed using transverse micro-radiography (TMR). The fluorine and calcium distributions in the carious lesion in each specimen were evaluated using the PIGE/PIXE system. From TMR analysis, there was a difference in caries risk between the two kinds of pH-cycling. Although the caries preventive effect of BS and FN was confirmed at low risk, the effect at high risk was confirmed for FN only. From the analysis of the fluorine uptake in the outer 200 μm of the lesion we concluded that there was no significant difference between the pH-cycling solutions. However, we found different fluorine concentrations in the enamel for the two FCMs. The decreased caries progression under high risk for FN indicated that an adequate amount of fluorine supplied from the material is required at higher caries risk. It was confirmed that the caries preventive effect of FCM depends on the caries risk. The fluorine analysis of teeth under various pH-cycling conditions gives information to evaluate the caries preventive effect of fluoride-containing materials according to the caries risk.     

A new mapping acquisition and processing system for simultaneous PIXE-RBS analysis with external beam

The combination of ion beam analysis techniques is particularly fruitful for the study of cultural heritage objects. For several years, the AGLAE facility of the Louvre laboratory has been implementing these techniques with an external beam. The recent set-up permits to carry out PIXE, PIGE and RBS simultaneously on the same analyzed spot with a particle beam of approximately 20 μm diameter.A new mapping system has been developed in order to provide elemental concentration maps from the PIXE and RBS spectra. This system combines the Genie2000 spectroscopy software with a homemade software that creates maps by handling acquisition with the object position. Each pixel of each PIXE and RBS maps contains the spectrum normalised by the dose. After analysing each pixel of the PIXE maps (low and high energy X-ray spectra) with the Gupixwin peak-fitting software, quantitative elemental concentrations are obtained for the major and trace elements. This paper presents the quantitative elemental maps extracted from the PIXE spectra and the development of RBS data processing for light element distribution and thin layer characterization. Examples on rock painting and lustrous ceramics will be presented.     

In vivo PIXE-PIGE study of enhanced retention of fluorine in tooth enamel after laser irradiation

The presence of fluoride in tooth enamel reduces the solubility of hydroxylapatite by acid attack. Fluoride presence (even at low concentration) in the oral cavity is efficient against caries process. We propose a new approach of the explanation of the increase of fluoride retention in the tooth enamel when low power laser irradiation is applied after the treatment with fluoride gel (fluoridation). External beam PIGE measurements of fluorine on extracted teeth have been made in order to determine the best sequence of the operations. The laser irradiation after fluoride application is more efficient than the reverse procedure. This observation is in agreement with previous observations that the fluorine penetration in the enamel takes place first in the soft organic material present between the polycrystalline (prismatic) structure before being integrated in the crystalline composition of hydroxylapatite in order to produce fluoro-apatite. As those in vitro measurements do not reflect the whole process in the saliva, in vivo PIGE measurements have been also performed. We have demonstrated, by repeating the PIGE measurements (at least five times at various time intervals) that a significant increase of the fluoride retention took place even 18 months after the unique laser treatment. The complete experimental procedure is described: fluoride application, laser irradiation, PIGE measurements with 2.7 MeV protons (repeated measurements at the same place on the same tooth in order to follow the evolution) and safety tests before in vivo analyses.     

Nuclear microanalysis of tooth enamel from a community in the Western Cape,South Africa

Extracted teeth collected from a Black African community living in the Gugulethu suburb of Cape Town, South Africa were studied by nuclear microscopy. Analysis by PIXE (with 3.0 MeV protons) of permanent extracted incisor and molar teeth from males and females of different ages showed a homogeneous elemental profile distribution for iron, zinc and strontium, irrespective of gender and/or age. Fluorine content as determined simultaneously from the 110 keV gamma-ray yield from proton bombardment had a similar mean value (females: 1.8% by mass and males: 1.6% by mass) for both genders. However, the mean content of strontium for females (97 μg g⁻¹) was about 40% lower than that for males (69 μg g⁻¹). In addition, a sub-group of children showed a smaller standard deviation on the distribution of zinc and fluorine. Previous results on the trace elemental concentration of the enamel of molar teeth, showed a depletion of up to 50% by mass for strontium after 20 h of exposure in acidic solution. Although the strontium level for the African female group fits this profile it is not certain what the demineralization observed was due too.     

Mapping elemental distributions in submarine hydrothermal sulfide smokers using proton induced X-ray emission

PIXE analysis using a 3 MeV proton beam on the CSIRO Nuclear Microprobe was carried out on samples of four typical undersea sulfide chimneys from the Rogers Ruins and Fenway hydrothermal sites, PACMANUS field, Eastern Manus Basin, Papua New Guinea. The ability of PIXE to map the spatial association of trace elements within the sulfides across multiple mineralogical zones provides important insights into the mode of formation of structures and the nature of interaction between ～250 and 350 °C hydrothermal fluids and 3–4 °C ambient seawater within the chimney walls.     

Combined PIXE/PIGE and IBIL with external beam applied to the analysis of Merovingian glass beads

New improvements on our archaeometry line at the cyclotron of the Institute of Nuclear and Atomic Physics and of Spectrometry of the University of Liège have allowed the use of PIXE/PIGE and IBIL in-air for the analysis of cultural heritage objects. The extraction is performed through a 100 nm thick Si₃N₄ window. The detection set-up consists now of two X-ray and one γ-ray detectors, together with a fiber optic UV–visible spectrometer. This set-up has already been tested for the analysis of modern corundum [1] and is now adapted to the analysis of archaeological artefacts. In this work, we have used it to analyse 216 out of the 5000 Merovingian glass beads that come from the necropolis of Bossut-Gottechain (Belgium), one of the most important ever found in Belgium.The IBA analyses confirmed the typological division of different beads groups through chemical composition that gives us new insights on fabrication techniques of glass matrices and colorants.     

CdTe detector use for PIXE characterization of TbCoFe thin films

Peltier cooled CdTe detectors have good efficiency beyond the range of energies normally covered by Si(Li) detectors, the most common detectors in PIXE applications. An important advantage of CdTe detectors is the possibility of studying K X-rays lines instead the L X-rays lines in various cases since CdTe detectors present an energy efficiency plateau reaching 70 keV or more. The ITN CdTe useful energy range starts at K-K_α (3.312 keV) and goes up to 120 keV, just above the energy of the lowest γ-ray of the ¹⁹F(p, p’γ)¹⁹F reaction. In the new ITN HRHE-PIXE line, a CdTe detector is associated to a POLARIS microcalorimeter X-ray detector built by Vericold Technologies GmbH (an Oxford Instruments Group Company). The ITN POLARIS has a resolution of 15 eV at 1.486 keV (Al-K_α) and 24 eV at 10.550 keV (Pb-L_α1). In the present work, a TbCoFe thin film deposited on a Si substrate was analysed at the HRHE-PIXE system. The good efficiency of the CdTe detector at 45 keV (Tb-K_α), and the excellent resolution of POLARIS microcalorimeter at 6.403 keV (Fe-K_α), are presented and the new possibilities open to the IBA analysis of systems with traditionally overlapping X-rays and near mass elements are discussed.     

Micro-ERDA,micro-RBS and micro-PIXE techniques in the investigation of fish otoliths

Elemental distribution in the otolith of the fresh water fish burbot (Lota lota L.) collected in Hungary was measured with Elastic Recoil Detection Analysis (ERDA), Rutherford Backscattering Spectrometry (RBS) and as a complementary technique, Particle-Induced X-ray Emission (PIXE) with a focussed ion beam of 1.5 × 1.5 μm² spot size. The organic- and inorganic-rich regions of the otolith are distinguished and they are presented as hydrogen and calcium maps at depth regions of 0–70, 70–140 and 140–210 nm. The textured surface of the sample and its porosity were characterized from the effect on the RBS spectra. The oxygen and carbon PIXE elemental maps can also be used to identify the organic- and inorganic-rich regions of the otolith. The calcium map was found to be more homogeneous because the otolith structure is averaged in a larger depth. The trace elements Fe, Zn and Sr were detected only in very low concentration by micro-PIXE.     

Ion beam microanalysis of individual aerosol particles originating from Saharan dust episodes observed in Debrecen,Hungary

Approximately 50 episodes of Saharan dust intrusion have been observed by PIXE in the atmosphere of Debrecen, Hungary since 1991 [I. Borbély-Kiss, Á.Z. Kiss, E Koltay, Gy. Szabó, L. Bozó, J. Aerosol Sci. 35 (2004) 1205]. In order to separate dust particles of Saharan origin from local sources, and to follow the formation, ageing and evolution of particles originating from long range transport processes, individual dust particle analysis was carried out on the Debrecen ion microprobe.The samples were collected on polycarbonate filters at a rural site 50 km from Debrecen during the Saharan sand plume in November 1996.Quantitative elemental concentrations for elements Z ? 6 were determined using PIXE–PIXE and STIM analytical methods. Saharan dust particles were selected on the base of characteristic elemental ratios like Ti/Ca, Ti/Fe and Al/Ca. Major and trace element content and possible chemical composition of the selected particles were determined.Single particle analysis of Saharan dust particles will lead to a better understanding of their formation process during transport.     

GIC4117串列加速器外束PIXE/PIGE分析系统

本文介绍在北京师范大学GIC4117串列加速器上建立的外束PIXE/PIGE分析系统,和基于此系统的薄样品外束PIXE/PIGE定量分析方法。给出了2010年Teflon滤膜采集的361个气溶胶样品外束PIXE分析得到的各元素平均探测限和最低探测限,并同真空PIXE分析探测限进行了比较。利用标准样品给出了激发曲线不同坪区薄样品外束PIGE分析F和Na的探测限,通过测定¹⁹F(p, p′γ)¹⁹F激发的197 keV γ射线得到的F的探测限可达73.9 ng•cm^-2,Na的探测限可达198.9 ng•cm^-2。     

High Resolution and Differential PIXE combined with RBS,EBS and AFM analysis of magnesium titanate (MgTiO3) multilayer structures

Thorough structural characterization of deep laying thin film, including the inference of interdiffusion profiles is frequently a complex problem. The use of RBS/PIXE holistic approaches, already shown to represent a powerful method, sometimes faces difficulties if standard experimental procedures are used. In this work, following a series of ⁴He Rutherford backscattering and ¹H elastic backscattering experiments, carried out to study the influence of SrTiO₃ as a possible cladding layer between Pt/TiO₂/SiO₂/(1 0 0)Si substrates and MgTiO₃ films, a simple holistic RBS-PIXE is shown to be not enough for the solution of such a problem. Establishing of the Sr depth profile, was only possible after AFM, High-Resolution EDS PIXE and differential PIXE analysis were carried out. Results, problems faced and conclusions obtained are presented.     

PIGE analysis of magnesium and beryllium

In this work, we present an alternative method for PIGE analysis of magnesium and beryllium 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 ²⁵Mg(p,p′γ)²⁵Mg (E_γ = 585 keV) and ⁹Be(p,γ)¹⁰B (E_γ = 718 keV) reactions were employed. Calculated gamma-ray yields were compared, at several proton energy values, with experimental yields for thick samples made of inorganic compounds containing magnesium or beryllium. The agreement is better than 5%. Taking into consideration the experimental uncertainty of the measured yields and the errors related to the stopping power values, this agreement shows that effects as the beam energy straggling, ignored in the calculation, seem to play a minor role.     

Quality control of coins mint using PIXE and RBS analysis

PIXE and RBS analysis is used to investigate the elemental content of modern Lebanese coins, in order to control their minting quality. The coins of interest were 100, 250 and 500 Lebanese Lira (LL), which are mainly bulky metals with or without coated layer. Using 3 MeV protons, proton induced X-ray emission PIXE identified and quantified elements while Rutherford backscattering spectrometry RBS checked the thickness of the coated layer. Indeed, the combination of PIXE and RBS provides a powerful tool to investigate the elemental composition of coins, either modern or ancient. In addition, the experimental protocol was checked by analyzing some other coins of known composition, such as 1-euro and 2-euro.     

External scanning micro-PIXE for the characterization of a polycapillary lens: Measurement of the collected X-ray intensity distribution

We developed a PIXE detection system for the analysis of medium-light elements which exploits a weakly focusing polycapillary lens for the transmission of the X-rays emitted from the target material to a Silicon Drift Detector. The polycapillary lens efficiently collects X-rays, while prevents back-scattered protons from impinging on the detector chip, thus avoiding electronics perturbation and consequent quality loss of PIXE spectra. The system is optimized for the detection of X-rays in the energy range 1–10 keV, when the emission from the target is induced by MeV proton beams with size of the order of a few hundreds of micrometers.This work reports the results of the lens characterization in terms of X-ray collection spot, i.e. the area of the sample actually “seen” by the lens, and its dependence on the X-ray energy. The lens properties have been measured using the external scanning microbeam facility of the Tandetron accelerator at LABEC-INFN in Florence. The detection system was used to detect X-rays from a set of pure elemental standards with an incident 3 MeV proton beam focused to a size of about 30 μm scanning an area of 1.9 × 1.6 mm². By measuring the spatial distribution of characteristic X-rays from each given material, the collection profile of the lens at the corresponding X-ray energy was obtained. Using several standards, the behaviour throughout the range 1–10 keV was examined. The sensitivity of the lens collection profile on the lens-sample out-of-focus distance was also investigated.     

Erosion and re-deposition processes in JET tiles studied with ion beams

Plasma facing components in fusion reactor chambers will operate under extreme conditions. Among the processes with implications on the material lifetime are erosion and re-deposition due to plasma interactions.This work will address the behaviour of both JET divertor and outer poloidal limiters (OPL) under plasma irradiation. The limiters comprise about 50 pairs of tiles in a poloidal stack, each of which has a plasma facing surface about 25 mm (poloidal) by 350 mm (toroidal) and is about 50 mm thick. The divertor tiles are located at the bottom of the chamber and withstand high fluxes of radiation and heat. Standard carbon-fibre composite (CFC) tiles coated with a thin layer of W overlaid with a 10 μm layer of C were studied with RBS/PIXE to understand the erosion/re-deposition processes occurring in these regions of the reactor chamber. High resolution surface morphology was assessed through SEM with and without tilting of the sample. The retention of hydrogen isotopes in the tiles were studied combining NRA and ERDA techniques – this is mostly ²H from the fuelling gas, but ³H is also present as a result of ²H–²H fusion reactions, and ¹H coming from the atmospheric exposure.     

The Maia 384 detector array in a nuclear microprobe: A platform for high definition PIXE elemental imaging

Application of nuclear microprobe event-by-event data acquisition approaches to synchrotron elemental imaging is at the heart of the design of a large energy-dispersive detector array called Maia, under development by CSIRO and BNL for SXRF elemental imaging on the X-ray microprobe. A new project is aimed at harnessing this development to provide high throughput PIXE imaging on the CSIRO Nuclear Microprobe. Maia combines a 1.2 sr solid-angle 384 detector array, integrated scanning and real-time processing including spectral deconvolution of full-spectral data. Results using a Maia prototype demonstrate the potential using SXRF application data with elemental images of up 100 M pixels.     

Challenges and opportunities in high-precision Be-10 measurements at CAMS

We determined the overall efficiency for ¹⁰Be of the high-intensity LLNL modified Middleton cesium sputter source in combination with the CAMS FN mass spectrometer. BeO^? ionization efficiency is >3%. Charge exchange efficiency including transmission through the tandem for 7.5 MeV Be⁺³ is ～34%, resulting in a total system efficiency of just over 1%. At this efficiency and with very low backgrounds, we estimate our detection limit to be ～1000 ¹⁰Be atoms. Cathodes prepared with only ～80 μg of ⁹Be show only an ～33% reduction in ⁹Be beam current compared to a sample with ～200 μg. These same samples, prepared from 07KNSTD1032 standard material, contained 1 × 10⁷ and 5 × 10^{6 10}Be atoms and exhibited similar ionization and total system efficiency. These results demonstrate the feasibility of pursuing applications that require precise measurement of samples with low ¹⁰Be concentrations and/or small sample size.     

Angular and lateral spreading of ion beams in biomedical nuclear microscopy

Nuclear scattering from target atoms gives rise to a spatial broadening of energetic ion beams penetrating matter. The spatial broadening of the ion beam presents an ultimate limit to the resolving power that can be achieved in nuclear microscopy methods. The pressing of the attainable resolution limit in biomedical nuclear microscopy to dimensions approaching 10 nm, or so, implies the fundamental limitation from ion-target scattering will become increasingly significant. This effect has been investigated by a combined analytical and numerical computational approach to determine the extent and how single and multiple scattering processes limit the resolution for analysis with 2 MeV ⁴He and ¹H ions of realistic biomedical samples. The cases studied were direct-Scanning Transmission Ion Microscopy (direct-STIM), Particle Induced X-ray Emission (PIXE) studies of 20 μm tissue sections and in vivo single-ion irradiation of cells.     

Weldability of neutron irradiated austenitic stainless steels

Degradation of weldability in neutron irradiated austenitic stainless steel is an important issue to be addressed in the planning of proactive maintenance of light water reactor core internals. In this work, samples selected from reactor internal components which had been irradiated to fluence from 8.5 × 10²² to 1.4 × 10²⁶ n/m² (E > 1 MeV) corresponding to helium content from 0.11 to 103 appm, respectively, were subjected to tungsten inert gas arc (TIG) welding with heat input ranged 0.6–16 kJ/cm. The weld defects were characterized by penetrant test and cross-sectional metallography. The integrity of the weld was better when there were less helium and at lower heat input. Tensile properties of weld joint containing 0.6 appm of helium fulfilled the requirement for unirradiated base metal. Repeated thermal cycles were found to be very hazardous. The results showed the combination of material helium content and weld heat input where materials can be welded with little concern to invite cracking. Also, the importance of using properly selected welding procedures to minimize thermal cycling was recognized.