An automated neutron activation system for short-lived nuclides

The present paper describes an attempt to create a reliable and easy to use system for neutron activation with short-lived nuclides, suitable to be used with several irradiation and counting procedures in instrumental neutron activation analysis (INAA) at the Portuguese Research Reactor. This system can become very useful for a large community within LNETI, as well as other national institutes and universities, particularly for those involved in studies where the analysis of a large number of samples is required. Selenium determination has been performed, through the short-lived nuclide^77mSe, as an example of the reliability of the system.     

Validation of a loss-free counting system for neutron activation analysis with short-lived indicators

The use of loss-free counting systems makes possible the exact correction for pile-up and dead-time losses during counting of a mixture of short-lived radionuclides even at very high count rates. However, counting statistics cannot be calculated by taking into account only the Poisson distribution of the incoming -quanta, such as is done in existing computer programs for -spectrometry. At moderate count rates Müller statistic was found to account for the observed variability between duplicate countings; however, at higher count rates the variability of weighing factors was found to be significant in comparison with the Müller statistic. While counting statistics could not be correctly estimated for short-lived species, experiments showed excellent accuracy for initial dead times up to 90%.     

An automatic data acquisition and handling system for activation analysis

An automatic measurement and data handling system for activation analysis is described. The system comprises five automatic -spectrometers with sample changers, a central computer with four workstations and two communication networks, one to connect the gamma-spectrometers with the central computer and another to provide communication from the workstations to the central computer. The software comprises programs for control of the -spectrometers, communication between the different units, data handling and storage, interpretation of -spectra, calculation of element concentrations and creating reports.     

An automatic NAA analyzer for short-lived nuclides

An automatic activation analyzer with sample changer, pneumatic transfer system and fast pulse counting with real time pulse pile-up and dead time compensation is described. Transfer times between 80 and 300 ms from irradiation position to measurement station can be obtained. Counting losses are corrected within 10% up to total count rates of 120 kc/s.     

Fast-neutron activation analysis with short-lived nuclides

At the GKSS Research Center Geesthacht, a new 14 MeV activation facility—a 5·10¹² n/s neutron generator combined with a fast rabbit system (KORONA)—is being installed. Homogeneous neutron flux at a level of 5·10¹⁰ n·cm⁻²·s⁻¹ and sample transfer times of 140 ms to a 16m distant detector station are characteristic features of the facility described in the paper. With special consideration of short-lived nuclides and including cyclic activation, the analytical prospects with the intense neutron source are discussed, and sensitivities for 78 elements are presented.     

On the use of a dead-time meter for pile-up corrections

Correction for pile-up losses in the amplifier is possible by the dead-time fraction indicator of the ADC in case of long-lived radionuclides. If the dead-time meter has been calibrated, an accuracy of 1.5% is feasible up to a dead-time fraction of 25%. The precision decreases from 1.5% at 10% dead-time fraction to 3% at a deadtime fraction of 30%.     

Instrumental dead-time and its relationship with matrix corrections in x-ray fluorescence analysis

The relationship between instrumental dead-time and the self-absorption coefficients, α_ii, in x.r.f. matrix correction by means of influence coefficients, is not generally recognized but has important analytical consequences- Systematic errors of the order of 1% (relative) for any analyte result from experimental uncertainties in instrumental dead-time. Such errors are applied unevenly across a given range of concentration because the error depends on the calibration standards and on the instrumental conditions used. Refinement of the instrumental dead-time value and other calibration parameters to conform with influence coefficients determined elsewhere assumes exact knowledge of dead-time of the instrument used originally, and quite similar excitation conditions and spectrometer geometry for the two instruments. Though these qualifications may not be met, adjustment of any of the parameters (dead-time, reference concentration, background concentration, self-absorption and other influence coefficients) can be easily achieved.     

Development of an automatic system for neutron activation analysis

An automatic measurement system for activation analysis has been developed at the La Reina Nuclear Center of the Chilean Nuclear Energy Commission. A gamma-ray spectrometer equipped with an automatic sample changer is linked to an IBM-compatible PC/AT. The peripheral devices are interconnected and suitable software for routine operation have been prepared. The computer handles solenoid valves and microswitch sensors. The gamma-spectra are stored in the hard disk and later transferred to a main frame computer where all the information is processed to obtain final results. The system is in full operation and the operation manuals that have been prepared allow it to be used by people who are not trained in activation analysis.     

Selection of short-lived isotopes for activation analysis with respect to sensitivity

During the last decade the use of short-lived isotopes in activation analysis has exploded, owing to the application of high resolution gamma-ray spectrometry. Complex spectra can in fact be resolved without the need for chemical separations. The application of cyclic activation-counting enables the use of isotopes with half-lives below 10 seconds. These short-lived isotopes can be produced by different activation processes. As neutron sources one can distinguish reactors, generators for 14 MeV or high energy machines such as cyclotrons and isotopic neutron sources. High energy photons can be produced by interaction of an energetic electron beam with a target, giving rise to an intense bremsstrahlung spectrum with maximum energy from 10 up to 70 MeV. While these photons induce several types of threshold reactions, lower energetic photons are used for resonance activation producing metastable isomers. More and more also charged particles (p, d,³He, α) are being used as projectiles to produce radioactive isotopes that can be measured in activation analysis. In the present paper a concise compilation is made of the nuclear reactions, applicable in activation analysis of minor or trace constituents using gamma emitting isotopes with half-lived smaller than 1 hour. Activations of all naturally occurring elements, except the noble gases, with Z values ranging from 9 to 92 have been considered. The reactions resulting in the most sensitive gammaspectroscopic determinations have been selected and are tabulated per element, together with the appropriate cross section and the resonance integral if significant for neutron reactions, the cross section at the giant resonance energy for the photon and at the maximum of the excitation function for the charged particle reactions and the threshold energy for all threshold reactions. For each isotope produced the half-life and the major gamma-ray energy is given. Finally calculated or experimental sensitivities have been compiled from a number of references, as the emission rate per second of the most intense gamma-ray, at the end of a 1 minute irradiation under well-defined circumstances for 1 microgram of the element. When cyclic activation has been applied it is indicated. These data are provided for more than 200 nuclear reactions. It appears that the majority of the 70 elements constacred can in some way be determined with a high sensitivity after such a short irradiation. Only for the elements Tm and Tb no reaction yielding a short-lived isotope with a reasonable sensitivity could be found. Both elements can however very sensitively be determined after a longer neutron irradiation. For a number of elements activation analysis by means of the middle-long-lived isotopes (2 hours to 3 days) is the most sensitive even after a 1 minute irradiation and immediate count (Mn, Ga, As, Sr, Ru, La, Eu, Ho, Lu, Os and Au). But for all other elements the highest gamma emission rate results from isotopes with half-lives shorter than 1 hour. Extremely high counting rates are obtained after thermal reactor neutron activation for Na, Sc, V, Co, Se, Rh, Ag, In, Eu, Dy, Er and Hf. For a number of elements the selectivity of the analysis can however largely be enhanced by irradiation under Cd-cover. High σ₀ ratios exist in fact for activation of medium and high Z elements such as Nb, Rb, Rh, Sn, Sb, Ba, Ce, Lu, Ta, Os, Hg and U. For some elements activation with reactor fission neutrons or 14 MeV neutrons provides an interesting sensitivity for a threshold reaction or the production of an isomer (F, Si, P, Cl, Ca, Cr, Se, Y, Ba, Ce, Pr, Bi, Pb). Cyclic activation and counting of very short-lived isotopes has been applied advantageously in the ng to μg range for a number of elements. Also cyclic activation with a 14 MeV generator has recently been studied. Low energy photon activation analysis allows selective production of metastable isomers of Se, Br, Ag, Er, Hf, Ir and Au, while high energetic photon production analysis yields high specific activities for elements such as K, Cr, Se, Br, Mo, Pr, Nd, Ho and allows interesting determinations of Mg, Cl, Si, Cr, Fe, Zr and Pb. Also charged particle activation can be used with surprisingly high sensitivity for some medium and high Z elements (Cr, Y, Se, Br, Zr, Mo, La, Ta, V). The intensity of the irradiation is in these cases mostly only limited by the properties of the sample itself, such as heat transfer and matrix activity. Examples of the compilation will be discussed and applications shown.     

New perspectives for very short-lived neutron activation analysis

Recent attempts to improve the performance of very short-lived neutron activation analysis are reviewed. It is shown that the combination of an intense cold neutron beam from a research reactor with a beam chopper offers higher signal-to-background ratio, more accurate timing and much simpler sample handling than conventional cyclic activation analysis. Application of a digital spectrum analyzer in data list mode allows for easy determination of the half-life. Hence, time-resolved activation analysis utilizing energy and time information becomes practical. This revised version was published online in July 2006 with corrections to the Cover Date.     

A correction for dead-time losses in γ-ray spectrometry for a mixture of short-lived radionuclides

A simple procedure for the correction of residual dead-time losses in γ-ray spectrometry of mixtures of short-lived radionuclides is given. It is based on the value of the total deadtime at the beginning of the measurement and three constants which are characteristics for a given matrix. The application to the instrumental neutron activation analysis of fluorine and sodium in bone is given as an exaple.     

Remote system for the mass production of short-lived radioisotopes in a cyclotron. Development of the system and radioisotope production

A system was developed for producing short-lived radioactive substances (11CO, 11CO2, 13NN, 13NH3, 18F-, 62Zn2+, 123I-, etc.) on a scale enough for clinical use, which could also be used for analyzing them rapidly and for investigating their production methods, with less received dose by workers. The system enabled us to produce remotely several tens mCi of of short-lived radioactive susbtances readily usable for clinical diagnosis, continuosly for radioactive gases, 11CO, 11CO2 and 13NN, or repeatedly at short intervals for radioactive aqueous solutions of 13NH3, 18F-, etc. Employing this system, the average received dose per month was reduced considerably.     

Trends in instrumentation for activation analysis of short-lived nuclides

This paper reports on the last year's two major activities of our nuclear instrumentation group it the field of high rate and high resolution gamma spectrometry which were mainly devoted to the needs of activation analysis of short-lived nuclides. The first of the projects was the completion of a state-of-the-art spectrometry system for very high counting rates which has been installed at the fast inrradiation and transport facility of the TRIGA reactor and now is the main instrument for the short-lived work of our radiochemistry group. Based on a laboratory-designed gated integrator pulse processing system and equipped with an Ortec Gamma-X detector of 20% relative efficiency with cooled FET and transistor reset preamplifier, it exhibits a basic resolution of 2.3 keV at 1332 keV which at a counting rate of 1.1 million cps of⁶⁰Co degrades to 3.4 keV. An essential feature of the system is a novel quantitative pileup rejector of the pulse counting type which has been specially designed for high rejection efficiency and at the same time, for the reliable exemption of valid events, and thus is a necessary prerequisite for quantitative real-time correction of counting losses by means of the Virtual Pulse Generator method. The second project included the successful implementation of the novel Preloaded Filter Technique (applied for patent), a new method for high resolution and high throughput processing of nuclear detector signals which, in contrast to conventional techniques, does not rely on a fixed pulse processing time per event which up to now was the main reason for pulse pileup and limited throughput, but, at the latest, terminates the filtering process of an individual event at the instant of arrival of the next event which results in optimized throughput and, at the same time, in a self-adapting, counting rate dependent shaping time. To that aim, the delta-noise filter of the system must be preloaded with the best estimate of the final result of the filtering process which is simply the unfiltered signal amplitude, to make sure that at the instant of termination of the filtering process the output of the filter deviates from the final value not more than by the decaying noise amplitude. Complemented by counting rate dependent step-noise filtering, this technique made possible the creation of a spectrometry system for all purposes which at low to medium counting rates is comparable to the best of the semi-Gaussian amplifiers and at high counting rates to the gated integrator. An experimental implementation of the Preloaded Filter combined with an Ortec Gamma-X detector of 15% relative efficiency resulted in a basic resolution of 1.9 keV at 1332 keV at a counting rate of 5000 cps slowly degrading to 3.2 keV at a counting rate of 650 000 cps of⁶⁰Co.     

A software counting loss correction method for neutron activation analysis with short-lived radionuclides

A method has been developed for the correction of counting losses in NAA for the case of a mixture of short-lived radionuclides. It is applicable to systems with Ge detectors and Wilkinson or successive approximation ADC's and will correct losses from pulse pileup and ADC dead time up to 90%. The losses are modeled as a constant plus time-dependent terms expressed as a fourth order polynomial function of the count rates of the short-lived radionuclides. The correction factors are calculated iteratively using the peak areas of the short-lived radionuclides in the spectrum and the average losses as given by the difference between the live time and true time clocks of the MCA. To calibrate the system a measurement is performed for each short-lived nuclide. In a test where the dead time varied from 70% at the start of the measurement to 13% at the end, the measured activities were corrected with an accuracy of 1%.     

An automated activation analysis system

An automated delayed neutron counting and instrumental neutron activation analysis system has been developed at Los Alamos National Laboratory's Omega West Reactor (OWR) to analyze samples for uranium and 31 additional elements with a maximum throughput of 400 samples per day. The system and its mode of operation for a large reconnaissance survey will be described.     

Use of very short-lived nuclides in nondestructive activation analysis with a fast shuttle rabbit

The use of 0.80 sec^207m Pb for the nondestructive determination of lead is described. The 0.570 MeV gamma-ray activity is measured, and corrections are made to allow for the rapid decrease of the dead-time during the measurements. A sensitivity of about 1400 cps/mg Pb and a precision of ±4 % were obtained with a neutron flux of 5·10¹² n·cm^?2·sec^?1. The influence of possible interferences was studied. The fast shuttle rabbit used in this type of analysis is described.