The development of nuclear microprobe techniques for the spatial determination of13C and13C/12C ratios

Sensitive and selective nuclear reaction methods have been sought for the nuclear microprobe measurement of the spatial distributions of¹³C and¹³C/¹²C ratios. The¹³C(α, n)¹⁶O reaction, with neutron detection, is the most selective for¹³C, and has a sensitivity of ca. 100 ppm. The reactions¹³C(d, p)¹⁴C and¹²C(d, p)¹³C, with proton detection, are the most sensitive for the simultaneous measurement of¹³C and¹²C, with detection limits of 30 and 2 ppm respectively. Less sensitive alternative reaction pairs are;¹³C(³He, p)¹⁵N and¹²C(³He, p)¹⁴N;¹³C(d, nγ)¹⁴N and¹²C(d, pγ)¹³C;¹³C(³He, pγ)¹⁵N and¹²C(³He, pγ)¹⁴N. The conditions governing their use, particularly light element interferences, are detailed.     

Determination of relative and absolute abundance of stable nitrogen isotopes by proton induced nuclear reactions

Thick-target yield of γ-rays emitted in the reactions¹⁴N(p,p′γ₁)¹⁴N and¹⁵N(p,αγ₁)¹²C were measured as a function of bombarding energy in order to select the conditions favoring the employment of these reactions in nitrogen isotopic analysis. The applicability of these reactions in the determination of relative as well as absolute nitrogen isotopic abundances was demonstrated at 4.3 MeV bombarding energy. Supported in part by the International Atomic Energy Agency, Vienna, Austria.     

Investigation of water diffusion into quartz using ion beam analysis techniques

Diffusion of water into quartz was studied by measuring H and ¹⁸O concentration profiles in surface layers of quartz samples treated hydrothermally in the range of 125° C to 200° C. Sample surfaces were orientated normal to the c-axis. The measurements were performed using the nuclear reactions ¹H(¹⁵N,αγ)¹²C and ¹⁸O(p,α)¹⁵N. The diffusion profiles have widths of up to 500 nm. Diffusion rate constants derived from the profiles are in the range of 10^–15 cm²/s to 10^–18 cm²/s and show a distinct temperature dependence, yielding a rough estimate of about 60 kJ/mole for the activation energy. Received: 24 June 1996 / Revised: 20 January 1997 / Accepted: 22 January 1997     

The use of charged particle bombardment for studying oxygen self-diffusion in oxides

The various nuclear techniques which have been used to study oxygen self-diffusion in oxides are discussed. Results are given for measurements using resonance capture in the¹⁸O(p, α)¹⁵N and¹⁸O(p, γ)¹⁹F reactions and the different techniques are compared.     

Recent developments in the analytical application of prompt spectrometry

A survey of the possibilities of analysis by alpha-induced prompt gamma-ray spectrometry is reported for 57 elements at a bombarding energy of 5 MeV. Additional data obtained at 11 and 16 MeV are given. Interference-free sensitivities are presented. The use of the position sensitive detector is introduced to overcome problems such as occur in prompt alpha spectrometry from (p, α) reactions. The technique is illustrated by studies on the reaction¹⁹F(p, α)¹⁶O and severely tested for boron analysis using the reaction¹¹B(p, α)⁸Be and measuring the α₀ and α₁ groups.     

Comparison of the3He/16O and1H/18O prompt nuclear reactions for lattice location measurements of oxygen in niobium

Experimental data are presented for comparison of the determination of oxygen by the¹⁶O(³He, p)¹⁸F,¹⁶O(³He, α)¹⁵O and¹⁸O(p, α)¹⁵N prompt nuclear reactions, and of their use in the lattice location, by the ion-channelling technique, of oxygen atoms in single crystal targets of elements such as niobium, where oxygen contents of ≈0.1 atomic % or more can be obtained. Both reaction cross-sections and lattice-defect production rates are considered in the comparison. Details are given of an arrangement for automatic crystallographic angular scanning of nuclear reaction and backscattering yields in channelling/lattice location measurements.     

Industrial production and purification of <Superscript>32</Superscript>P by sulfur irradiation with partially moderated neutron fluxes and target melting

Target purification of S_α is carried out by distillation at 444±2 °C under N atmosphere and diluting the vapors in CS₂. The solution is filtered through fiberglass, Teflon and cellulose to obtain S_α by CS₂ evaporation. Once 30 g of this target are irradiated with fast neutron fluxes from 4.5 to 7.4·10¹² n·cm⁻²s⁻¹ from 6 to 12 hours, the nuclear reaction ³²S(n,p)³²P takes place. So, the irradiated S_α sample is placed in a Pyrex container situated inside a furnace as the most important piece of equipment in one aluminum and Lucite glove box. The distillation of irradiated sulfur takes place at 444±2 °C under N atmosphere during 1–2 hours. The vapors are connected to a sulfur diluter containing 20% CS₂ aqueous solution, followed by an activated carbon filter and the two similar additional sulfur diluters. Once cooled, the distillation chamber keeps the radioactive, carrier-free ³²P stuck to the wall. Then 25–50 ml of 0.1N HCl acid was injected by suction and heated again at 110±2 °C during 1 hour. The corresponding chemical reaction takes place and the labeled H₃ ³²PO₄ solution is produced. In such a way, industrial production of ³²P labeled molecules has started in Mexico, with an initial production of 3700–5550 MBq per week.     

Amorphous semiconductor thin films characterization by nuclear microanalysis

A review is presented summarizing the specific nuclear microanalysis methods applied in our laboratory to study amorphous semiconductor thin films. For backscattering, ∼3 MeV Li ions are applicable when depth resolution and sensitivity are required while up to 8 MeV α-particles allow larger depths to be probed and elemental interferences to be solved. These features are predominant for diffusion studies between metal electrodes and chalcogenide films. On the other hand hydrogen profiling using the¹H(^{1 5}N, αψ) resonant nuclear reactions is described and analytical problems associated with its use are discussed. Applications to the elaboration conditions of hydrogenated (a)Si is developed. Work supported by C.N.R.S. (A.T.P. Materiaux 2726 and Photovoltaique A 651 3865) and the C.E.A.—D.A.M. (contract No 1350)     

Carbon isotope mass spectrometry in doping control

A procedure that makes it possible to establish the origin of endogenous steroids present in human urine by the determination of the ¹³C/¹²C carbon isotope ratio is described. A combination of solid-phase and liquid-liquid extraction, as well as semipreparative liquid chromatography, was used to separate fractions containing testosterone, 5α- and 5β-androstane-3α, 17β-diols, androsterone, ethiocholanolone, 5β-pregnane-3α, 20S-diol, and 16(5α)-androstene-3α-ol. More than 100 samples were analyzed by gas chromatography coupled with isotope mass spectrometry. The resulting values of ¹³C/¹²C were statistically processed, and the ranges required for the interpretation of the results were found. The procedure was certified and accredited in accordance with ISO 17025 requirements.     

Observation of a Doppler broadening of the 4438 keV gamma-line of12C in processes12C(n,n′γ)12C and9Be(α, nγ)12C

A Doppler broadening is described of the 4438 keV spectral gamma-line observed by means of a Ge(Li) detector during the deexcitation of nuclei of¹²C in an inelastic scattering¹²C(n, n′γ)¹²C using an²⁴¹Am−Be source as well as during the reaction⁹Be(α, nγ)¹²C taking place in the Am−Be source. The FWHM of the spectral line is equal to (90±4) keV in the latter reaction and (64±8) keV in the former process. Experimental values agree well with theoretical ones. Presented at the Instrumental Activation Analysis Conference, IAA 79, June 4–8, 1979, Klučenice, Czechoslovakia.     

Yields and average cross sections of recoil charged particle induced reactions on11B,12C,13C,14N,16O and18O

The yield and average cross section for the reactions¹¹B(p, n)¹¹C,¹²C(p, )¹³N,¹³C(p, n)¹³N, ₁₂ ¹² C(d, n)¹³N,¹⁴N(p, )¹¹C,¹⁶O(p, )¹³N,¹⁶O(d, n)¹⁷F,¹⁶O(t, n)¹⁸F, and¹⁸O(p, n)¹⁸F have been measured in different compounds. The charged particles were created in the samples themselves either through recoil by scattering of 14 MeV neutrons off hydrogen and deuterium, or by the (n, t) reaction on⁶Li using thermal neutrons. The yields of reactions¹²C(d, n);¹⁶O(p, );¹⁶O(t, n) and¹⁸O(p, n) have been measured using proton, deuteron and triton spectra generated by 14 MeV neutrons in the reactions D(n, p)2n;⁶Li(n, d);⁷Li(n, d) and¹⁰B(n, d);⁷Li(n, t) and¹⁰B(n, t), respectively.     

Determination de la fonction d'excitation de la reaction nucleaire1H(15N, α γ)12C entre 6 et 14 MeV

Thick targets (mica) and thin hydrogen layers obtained by ionic implantation of protons in silica are used to establish the excitation function of the nuclear resonant reaction¹H (¹⁵N, α γ)¹²C. Two main resonances in the energy gap explored were observed. Their FWHM and the cross section at E_R are specified. The experimental conditions required and the performances allowed, using this reaction to determine hydrogen depth profiles in the near surface region of solids, are presented. Examples concerning borosilicates, leached in aqueous medium, are given.      

Influence of the Native Oxide Layer on the Silicon Surface During Initial Stages of Nitridation

 Thin SiO₂ layers were produced by thermal oxidation of Si wafer material. To study the effect of nitridation on the oxide layers, the specimens were nitrided in a furnace at high temperature. Non-destructive ion beam analysis was performed to determine changes in the elemental concentrations and depth profiles of the major components. In particular, N and O concentrations were measured using the non-resonant nuclear reactions ¹⁴N(d, α)¹²C and ¹⁶O(d, p)¹⁷O, respectively. To obtain depth profiles of the as-prepared and nitrided specimens, the samples were measured with RBS and heavy ion elastic recoil detection analysis. The ion beam analyses revealed an increase in thickness of the SiO₂ layers with temperature. The specimens nitrided at 1200 °C were almost free of N. Surface topology investigations with scanning electron microscopy revealed concentric annular artificial patterns at the surfaces. In the centre of the pattern, only silicon was measured. Additionally, a band consisting of Si, O, and N surrounding the pattern was discovered. The findings are in agreement with specimens prepared at higher temperatures. Received June 19, 2000. Revision December 9, 2000.     

A compilation of charged particle production cross-sections by 14 MeV neutrons for Nb and Mo isotopes

A compilation of the cross sections (n, p), (n, n′ p), (n, α) (n, n′ α) and (n,³He) for⁹³Nb,^{92,95,96,97,98,100}Mo by 14 MeV neutrons is presented in the form of a table containing the results of nearly 70 different measurements, mainly obtained by activation analysis. Brief assessments of the experimental methods and the data status are given.     

Preparation of carbon-11 labelled acetate and palmitic acid for the study of myocardial metabolism by emission-computerised axial tomography

Methods have been developed for the labelling of acetate and palmitic acid with the positron-emitting radionuclide,¹¹C (T=20.4 min). Labelling was achieved via carbonation of the appropriate alkyl magnesium bromide (methyl magnesium bromide or n-pentadecyl magnesium bromide) with¹¹C-labelled carbon dioxide produced by the¹⁴N(p, α)¹¹C nuclear reaction. The radiochemical yield and speed of each method of labelling are such that a radiochemically pure product is obtained in injectable form and in activity (>10 mCi) suitable for the study of myocardial metabolism by emission-computerised axial tomography. High pressure liquid chromatography and thin layer chromatography were used to assess the radiochemical purity of each radiopharmaceutical. The specific activity of¹¹C-labelled acetate was estimated by an enzymic procedure to be greater than 0.5 Ci/μmole.     

An electroconductivity study on degree of counterion binding or dissociation of a-sulfonatomyristic acid methyl ester micelles in water as a function of temperature

 For a sodium salt of α-sulfonatomyristic acid methyl ester (14SFNa), one of the α-SFMe series surfactants, the differential conductivity (∂κ/∂C) _T , _P vs. square root of concentration (√C) was employed in order to determine not only CMC but also the limiting molar conductance (Λ⁰) and the molar conductance of micellar species (Λ^M). Based on the data of the degree of counterion binding to micelles (β) determined previously at different temperatures ranging 15–50 °C at every 5 °C, the experimental values of the degree of dissociation (ionization) of a micelle (α_EX) were calculated by regarding as α_EX=1−β. The ratio Λ^M/Λ⁰ corresponding to the ratio of slopes below and above CMC in the curve of specific conductivity (κ) vs. concentration (C), which has been often assumed to be the degree of ionization of micelles (α), was compared with the present α_EX. However, the ratio Λ^M/Λ⁰ (=α) was found to have a correlationship with α_EX (=1−β) as α_EX≈0.40×(Λ^M/Λ⁰), or strictly, α_EX=0.40 (Λ^M/Λ⁰)+0.08, indicating that the simple ratio of the slopes below and above CMC in κ vs. C curve is not true for α_EX=1−β. On the other hand, the method proposed by Evans gave a value closer to α_EX compared with the simple ratio. Received: 17 September 1996 Accepted: 8 April 1997     

Light elements analysis and application to glass industry

Nuclear reactions induced on light elements by low energy deuterons are investigated. Differential cross-sections for¹⁰B(d, β₀)⁸Be,¹⁰B(d, β₁)⁸Be,¹²C(d, p₀)¹³C,¹⁴N(d, β₀)¹²C,¹⁴N(d, β₁)¹²C,¹⁶O(d, p₀)¹⁷O,¹⁶O(d, p₁)¹⁷O and¹⁶O(d, β₀)¹⁴N reactions are measured between 0.5 and 3 MeV at an observation angle of 135° with respect to the incident beam. Possible application of these reactions to the measurement of surface concentration is considered—Special emphasis was given on nitrogen determination in order to study nitrogen concentration in industrial glasses. Surface nitrogen repartition on glass, origin of nitrogen, influence of oxidizing and reducing conditions and glass structure are discussed.     

Measurement of neutron-induced activation cross sections of lanthanum at 14.8 MeV

Cross-sections for (n,p), (n,α), (n,n′α), (n,t) and (n,2p) reactions have been measured on ¹³⁹La isotope at the neutron energy 14.8 MeV using the activation technique in combination with high-resolution gamma-ray spectroscopy. Neutrons were produced via the ³H(d,n)⁴He reaction using a solid tritium–titanium target. The neutron fluences were determined using the monitor reaction ²⁷Al(n,α)²⁴Na. The neutron energy in this measurement was determined by cross section ratios for the ⁹⁰Zr(n,2n)^89m+gZr and ⁹³Nb(n,2n)^92mNb reactions. Data are reported for the following reactions: ¹³⁹La(n,p)¹³⁹Ba, ¹³⁹La(n,α)¹³⁶Cs, ¹³⁹La(n,n′α)^135mCs, ¹³⁹La (n,t)^137mBa, and ¹³⁹La(n,2p)¹³⁸Cs. The cross sections were discussed and compared with experimental data found in the literature, and with the comprehensive evaluation data in ENDF/B-VII.0, JENDL-3.3, JEFF-3.1/A, and TENDL-2008 libraries.     

The elemental and isotopic determination of lithium by the coincidence measurement of complementary particles

The coincident measurement of both nuclear products at their complementary angles was used to determine⁶Li by the reactions⁶Li(d, α)⁴He and⁶Li(p, α)³He, and⁷Li by the reaction⁷Li(p, α)⁴He. Elemental lithium was determined in natural samples or samples of known isotopic composition. Isotopic analyses could be carried out over the entire range from 0 to 100 atom% with a relative standard deviation of about 4%. The CMCP technique is highly specific and effectively eliminates interference and background.     

Determination of fluorine by the spectrometry of prompt gamma-rays

The use, for analysis, of prompt gamma-rays excited by 5 MeV alpha-particles from the reactions¹⁹F(α,α′γ)¹⁹F,¹⁹F(α, nγ)²²Na and¹⁹F(α, pγ)²²NE, was studied. The precision of the analyses depended on the gamma-ray energy used for the measurement. Relative standard deviations were ±1.8, ±0.9 and ±1.3% using the 110-, 197- or 1275 keV gamma-rays. The method was tested with N. I. M. standard materials of calcium fluoride and fluorspar, and was used as a rapid method for the determination of fluorine in cements.