Use of the nuclear microprobe at the University of Arizona for the study of heavy metal deposition in rabbit renal tissue

Industrial wastes consigned to disposal sites frequently contain substantial amounts of heavy metals. We have successfully applied proton induced X-ray emission analysis (PIXE) in the conduct of heavy metal (Hg, Cd, Cr, As) toxicity studies using precision cut rabbit renal cortical slices. The large beam diameter (4000 μm) of the proton macroprobe at The University of Arizona Ion Beam Analysis facility allowed an overall concentration of the metal(s) of interest in the samples to be determined, but lacked the ability to resolve point concentrations in the tissue. The ability to locate these areas has now been made available to us with the addition of a rastering microprobe (μ-PIXE) to the facility. Studies now being conducted in our laboratory using this micro-technique include analysis of renal tissue taken from rabbits injected intraperitoneally with HgCl₂, K₂Cr₂O₇, and NaAsO₂. The small beam size (3 μm) and the ability to raster this beam over areas of up to 125 μm × 125 μm has allowed regional mapping of endogenous and non-endogenous metal concentrations and revealed trends in heavy metal deposition in in vivo treated renal tissue, significantly increasing the amount of information obtained from these animal studies using PIXE alone. The combination of small beam size, high resolution, and multi-element detection makes μ-PIXE a powerful tool for investigating the impact of non-endogenous metals on the kidney.     

Analysis of metallic pigments by ion microbeam

Metallic paints consist of metallic flakes dispersed in a resinous binder, i.e. a light-element polymer matrix. The spatial distribution and orientation of metallic flakes inside the matrix determines the covering efficiency of the paint, glossiness, and its angular-dependent properties such as lightness flop or color flop (two-tone). Such coatings are extensively used for a functional (i.e. security) as well as decorative purpose. The ion microbeam analysis of two types of silver paint with imbedded metallic flakes has been performed to determine the spatial distribution of the aluminum flakes in paint layer. The average sizes of the aluminum flakes were 23 μm (size distribution 10–37) and 49 μm (size distribution 34–75), respectively. The proton beam with the size of 2×2 μm² at Ljubljana ion microprobe has been used to scan the surface of the pigments. PIXE mapping of Al K map shows lateral distribution of the aluminum flakes, whereas the RBS slicing method reveals tomograms of the flakes in uppermost 7 μm of the pigment layer. The series of point analysis aligned over the single flake reveal the flake angle in respect to the polymer matrix surface. The angular sensitivity is well below 1 angular degree.     

Quadrupole-doublet with permanent magnets for proton beam focussing

For PIXE studies on inhomogeneous samples with medium spatial resolution of about 50 μm two quadrupole doublets with Co₅Sm pole pieces for focussing 2.0 and 2.5 MeV proton beams, respectively, have been designed and tested. Technical data and first results are presented.     

Analysis of lichen thin sections by PIXE and STIM using a proton microprobe

In order to better understand the distribution pattern of mineral elements in lichen tissues, thin sections (15 μm) of the foliose, vagrant soil lichen Xanthoparmelia chlorochroa were examined using proton microprobe Particle induced X-ray emission (PIXE). This technique was used to make two-dimensional scans, with 5 μm resolution, across tissue cross sections of the test species. Element maps for Si, P, S, Cl, K, Ca, Ti, Mn, Fe, Cu, Zn, and As have been prepared. Several elements are strongly localized in the element maps. PIXE data are complimented with STIM, light micrographs, and SEM images. Preliminary data suggest that nuclear microprobe techniques may be useful in elucidating element absorption and transport mechanisms in lichens.     

Research of Si and GaAs diode structures by Ion Beam Induced Charge (IBIC) collection

A Si pn junction diode and a GaAs Schottky diode were prepared for studying the basic mechanism of charge collection followed by high energy charged particle incidence in order to improve the resistance against single event upset. A 2 μm wide and 20 μm long rectangular Al electrode attached to a circular Al electrode with a 50 μm diameter was made on a 2.5 μm thick epilayer (minority carrier density 2 × 10¹⁵ /cm³). Both a Schottky electrode of Al (5 μm × 110 μm) and two ohmic electrodes of AuGe/Ni (110 μm × 110 μm) were made on a 2 μm thick epilayer (7.3 × 10¹⁵ /cm³) grown on a semi insulator GaAs substrate (1 × 10⁷ Ω cm). The internal device structure was examined by the IBIC (Ion Beam Induced Charge) method using a 2 MeV He⁺ ion microbeam. IBIC images clearly show an Al electrode, the SiO₂, and an epilayer. These results were then used to improve the qualities of the test diodes.     

On the accuracy of element concentrations and masses of micron sized samples determined with the Heidelberg proton microprobe

We have already tested the reliability of element-normalized PIXE (Proton Induced X-ray Emission) data on small (10–100 μm) particles that we routinely obtain with the Heidelberg proton microprobe. Thus, we here discuss the accuracy of quantitative results, i.e., absolute concentrations inferred from PIXE analyses of such particles. We investigated and reduced the effects of mechanical vibrations and of the instability of the electronic devices on the achievable minimum beam spot. We implemented into our computer code a mapping software for qualitative element distributions (PIXE) and quantitative mass images using STIM (Scanning Transmission Ion Microscopy). The STIM images determine the area density required to calculate from PIXE spectra the absolute element concentrations in thin samples. The accuracy of absolute PIXE concentrations is tested by measurements on 15 μm soda lime glass microspheres. Finally, the complete results of PIXE and STIM analyses of an interplanetary dust particle (IDP) are described.     

Study of basic mechanisms of semiconductor devices using ion beam induced charge (IBIC) collection

A change of wave form of current transients induced by a single heavy ion was investigated around a pn junction with 8 μm width and 10 μm length as a function of the ion incident position. Three pn junctions were made on a 3 μm thick Si epilayer (1 × 10¹⁶/cm³) grown on Si substrate and were in a line along an aluminum electrode with 10 μm spacing between the adjacent junctions. The elements of a pn junction array were irradiated with a 1 μm diameter 15 MeV C⁺ heavy ion microbeam spacing steps by 3 μm. At a bias voltage of − 10 V, 148, 91, and 54 fC were collected at the pn junction center, and at 3 μm and 4 μm from the edge of the electrode, respectively. Internal device structure was examined by IBIC (ion beam induced current) method by using a 2 MeV He⁺ ion microbeam. From the IBIC spectrum and the IBIC image, the charge collected from the open space by the diffusion process was observed in addition to the charge collected from the depletion layer of the pn junction.     

PESA as a complementary tool to PIXE at CTU Prague

Proton Elastic Scattering Analysis (PESA) is a simple convenient method for hydrogen analysis in thin samples. A Proton Induced X-ray Emission (PIXE) target chamber was equipped with a PIPS detector for detection of forward-scattered protons. One of the objectives was to perform PIXE and PESA analyses of air particulate targets simultaneously. Tests and calibrations were fulfilled mainly with Mylar foils 1.5–6.5 μm thick in the proton energy region between 1.35 and 2.3 MeV. The energy dependence of scattering cross section is different from the Rutherford formula. Comparison of PIXE/PESA analysis with the Guelph Scanning Proton Microprobe Laboratory at the University of Guelph, Canada on seven aerosol samples was carried out. The intercomparison results validated our PESA/PIXE quality assurance protocol. In addition, repeated measurements of Gelman Teflo^TM filters indicated a gradual increase of hydrogen content by 1 ng/cm² per 1 μC/cm² proton dose.     

The external beam microprobe facility in Florence: Set-up and performance

An external beam microprobe facility, based on a quadrupole doublet supplied by Oxford Microbeam Ltd, has been installed on a new beamline at the 3 MV single-ended Van de Graaff accelerator in Florence. The goal was to obtain a beam with a spot size on target of 10–20 μm and a current in the order of at least 1 nA, in order to allow PIXE, PIGE and RBS elemental analysis in air or in a helium atmosphere. The beam was extracted from the vacuum lines through a 0.1 μm thick Si₃N₄ window to minimise lateral straggling. The design goals have been successfully achieved; the measurements of the beam spot characteristics in vacuum as well as in air and in helium atmosphere, are here reported.     

The interaction of iron with molten uranium

The rate of penetration of Armco iron by molten uranium, U-34 at % Fe eutectic and U-77 at % Fe eutectic was investigated in the range of 740 to 1300° C. This was done in an effort to understand the mode of penetration of uranium-base fuels through iron-base claddings. The phenomenon of particular interest was a penetration rate reversal, i.e. decreasing rate with increasing temperature, between 1150 and 1244° C.

Penetration rates at 1150° C were found to be 760 μm/sec in uranium, 690 μm/sec in U-34 at % Fe and 5.5 μm/sec in U-77 at % Fe. At 1244° C these rates changed to 150 μm/sec in uranium, 130 μm/sec in U-34 at % Fe and 5.7 μm/sec in U-77 at % Fe. The study showed that the penetration rate is related to the rate and mode of formation of UFe₂. The rate changes correlate well with the phases of the U-Fe equilibrium diagram.     

Magnetic force microscopy studies on the magnetic ordering in organic materials induced by high-energy proton irradiation

In this study, ferromagnetic microstructures in highly oriented pyrolytic graphite and superparamagnetic spots in polyimide foils were created by 2.25 MeV proton microbeam irradiation and characterized using atomic and magnetic force microscopy. For this purpose, graphite samples were irradiated with cross-like patterns of 15 μm × 15 μm size using ion fluences in the range of (0.003–2.5) × 10¹⁸ cm⁻². The irradiated crosses showed strong magnetic signals and a complex domain structure in the magnetic images depending on the geometrical dimensions of the crosses. Furthermore, polyimide foils were irradiated with microspots and fluences in the range of (0.016–3.1) × 10¹⁹ cm⁻². Magnetic force microscopy shows very strong phase shifts in these irradiated areas.     

Microbeam RBS on flat panel displays

We have demonstrated the utility of microbeam-Rutherford BackScattering (μ-RBS) in spatially resolved studies of operational plasma effects on the interior surfaces of plasma flat panel displays manufactured by Photonics Imaging. The experiments were performed at the Sandia Nuclear microprobe using a 2.8 MeV He beam with an average beam spot size of less than 8 μm. The interior surface of the top panes of the flat panels is composed of approximately 800 nm of MgO on top of a 2000 nm thick PbO layer. μ-RBS of sample panels operated under varying conditions measured changes in the surface MgO film thickness due to plasma erosion and redeposition as accurately as ± 1.5 nm. The high accuracy in the MgO thickness measurement was achieved by inferring the MgO thickness from the shift of the Pb front edge in the RBS spectrum. An estimate for the thickness accuracy as a function of the acquired statistics is presented. The surface of the flat panels' bottom panes is also comprised of MgO on top of PbO. However, troughs 100 μm wide by 10 μm deep were partially filled with phosphor and cover the entire width of the surface. This leaves only 100 μm long sections of MgO within the trough exposed. Using μ-RBS, we were able to analyze the surface composition of these regions.     

Extraction efficiency of N(T1/2 = 9.96 min) atoms from a graphite target: comparison between off- and on-line obtained results

An off-line release study ¹³N(T1/2 = 9.96 min) produced by proton induced reaction on a graphite target (POCO-graphite EDM3, density = 1.84 g/cm³, grain size /t 3 μm) has been performed. The activation energy for the diffusion process is determined to be 6.15(16)×10⁵ J/mol. With this activation energy, extraction efficiencies for ¹³N are obtained at different temperatures and are compared to on-line measured extraction efficiencies.     

Size-fractionated aerosol composition during an intensive 1997 summer field campaign in northern Finland

A 12-stage small deposit area low pressure impactor (SDI) was used to collect size-fractionated aerosol samples during an intensive 1997 summer field campaign in northern Finland. The samples were analyzed for over 20 elements by PIXE, and some “difficult” elements such as As and Se could be quantified. The sea-salt and crustal elements had essentially a unimodal coarse size distribution with geometric mean aerodynamic diameter (GMAD) of about 4–5 μm. In one third of the samples, S showed only one mode in the fine size range, with GMAD of 0.4–0.5 μm. In the other samples, this fine S mode broke up into two modes, with GMADs of 0.3 and 0.6 μm, respectively. V, Zn, As, Se and Pb were mainly present in a single submicrometer mode, with GMAD of 0.4–0.5 μm for V and Se, and slightly larger (i.e., 0.6 μm) for the other three elements. The highest concentrations of S, V, Ni, Cu, Zn, As, Se and Pb were encountered in the SDI sample which had been collected in the period 14–16 July. During this sampling, the air masses came in from the west, but had recirculated over northern Scandinavia and passed over the Kola peninsula.     

Microbeam line with 1.5 MeV helium ions and protons at Osaka

A microprobe for Rutherford backscattering (RBS) and particle-induced X-ray emission (PIXE) measurements has been realized by focusing 1.5 MeV helium-ion or proton beams with a demagnification system consisting of piezo-driven objective slits and a magnetic quadrupole doublet. Minimum beam spot sizes of 1.3 × 2.2 μm² for helium ions and 2.2 × 4.0 μm² for protons have been achieved. The factors which may limit the minimum spot size are discussed using a Monte Carlo simulation procedure. Rutherford backscattering image mapping of 3-dimensional structures is demonstrated.     

Nuclear mubeams: Realization and use as scientific tool

A nuclear mubeam is an ion beam focussed down to a spot of only a few μm in diameter. If such a beam is surrounded by equipment for elemental analysis we have the nuclear muprobe (NMP) suited for elemental analysis with μm spatial resolution and detection limits of a few ppm. The beam focus is achieved by collimation to some 10 μm and further demagnification with the help of an appropriate lens system. The need to fabricate the mechanical parts to a very high precision and to avoid slit scattering at the collimators will be demonstrated and a guide to the optimal design will be given. The different ways of realization are illustrated. Applications in different fields of science are given and the availability of NMPs throughout the world illustrated.     

Beam heating and cooling of thick targets for on-line production of exotic nuclei

Calculations have been made of energy deposition distributions for “thick” targets (1 mole/cm²) employed in on-line production of exotic nuclei using the Monte Carlo based LAHET code system for high-energy charged particle transport. A variety of target materials and incident proton beam energies have been examined. For 600 MeV protons, the results are compared to those from a similar study reported in the literature. The agreement between the two studies for total energy deposition is reasonably good for monatomic targets, but the results differ in some details of the energy deposition distributions. Target cooling, both radiative and conductive, is examined to assess the suitability of existing target concepts exposed to bombardment by intense (up to 100 μA), energetic (500 MeV to 1.2 GeV) proton beams to produce exotic nuclei. Implications of cooling requirements to target material selection and design are discussed.     

Corrosion of steels with surface treatment and Al-alloying by GESA exposed in lead–bismuth

Corrosion tests were performed for T91, E911 and ODS (oxide dispersion strengthened) with surface treatment and Al-alloying by pulsed electron beam (GESA—GepulsteElektronenStrahlAnlage) in flowing lead bismuth eutectic (LBE) with an oxygen content of 10⁻⁶ wt% at 550 °C for 2000 h. The result was that the surface treatment by GESA led to a faster growing multiphase oxide layer which was very homogenous in thickness. After exposure of specimens to LBE, the average oxide layer at the surface was 14–15 μm thick for ODS, 19–20 μm for E911 and 8–22 μm for T91. No dissolution attack occurred. On the surface of the Al-alloyed specimens, thin protective alumina layers were observed at the places where FeAl was formed by the GESA process, otherwise multiphase oxide layers or corrosion attack were observed.     

Detailed mass size distributions of atmospheric aerosol species in the Negev desert, Israel, during ARACHNE-96

As part of the 1996 summer intensive of the Aerosol, RAdiation and CHemistry Experiment (ARACHNE-96), the mass size distribution of various airborne particulate elements was studied at a remote site in the Negev Desert, Israel. Aerosol collections were made with 8-stage PIXE International cascade impactors (PCIs) and 12-stage small deposit area low pressure impactors (SDIs) and the samples were analyzed by PIXE for about 20 elements. The mineral elements (Al, Si, Ca, Ti, Fe) exhibited a unimodal size distribution which peaked at about 6 μm, but the contribution of particles larger than 10 μm was clearly more pronounced during the day than during night. Sulphur and Br had a tendency to exhibit two modes in the submicrometer size range, with diameters at about 0.3 and 0.6 μm, respectively. The elements V and Ni, which are indicators of residual fuel burning, showed essentially one fine mode (at 0.3 μm) in addition to a coarse mode which represented the mineral dust contribution. Overall, good agreement was observed between the mass size distributions from the PCI and SDI devices. The PCI was superior to the SDI for studying the size distribution in the coarse size range, but the SDI was clearly superior for unravelling the various modes in the submicrometer size range.     

Study by PIXE method of trace elements transferred from prostheses to soft tissues and organs

Some metallic prostheses inserted in human hip undergo physico-chemical modification, a few years after their implantation. Tissues surrounding these prostheses are damaged by metallic element transfer. Surgeons in Clermont-Ferrand Hospital (France) recover tissues of abnormal coloration that were in contact with metallic implants. PIXE technique (particles induced X-ray emission) with a 400 μm proton beam and 3 MeV of energy is an efficient technique to analyze these tissues and to detect elements, which are transferred from prosthesis to tissues. PIXE analyses were carried at the CERI-CNRS Laboratory. We have applied this method to determine qualitatively and quantitatively trace elements migration from metallic implants to surrounding tissues and organs, like kidney, spleen, liver, lymphatic gland and lung.