Improved accuracy and robustness of NAA results in a large throughput laboratory by systematic evaluation of internal quality control data

The laboratory for INAA in Delft processes several thousands of samples per year for multielement determinations in a variety of matrices. Samples are measured on different spectrometers (using well-type and coaxial detectors), by different persons and using many different analytical protocols. All these results should be consistent with each other with respect to the degree of accuracy, i.e., the combination of trueness and precision. A rigorous internal quality control program has been implemented with automatic on-line evaluation. Annually an additional evaluation of the internal quality control results is carried out using statistical techniques. The Naji-plot approach has proven to be an important graphical tool since it provides direct insight in both trueness and precision. It is demonstrated that the degree of accuracy of the results obtained under the large variety of operational parameters is under constant improvement.     

Automation and Quality Assurance in the NAA Facilities in Delft

The facilities for instrumental neutron activation analysis in Delft are described. Technical details of the fast rabbit systems, the normal pneumatic rabbit system, the large sample facility and the various coaxial and well-type Ge-detector spectrometers and sample changers are given. The capacity of the facilities is in the order of 15,000 samples per annum for full multi-element analysis. The capacity of the fast rabbit systems for INAA for use with short half-life radionuclides is even larger. The facilities are accessible for use by scientists from other establishments and countries as well.     

A comparison of pulser-based analog and digital spectrometers

We have begun a program of updates to the instruments used by the Radiation Measurements Laboratory at the Idaho National Laboratory. This laboratory supports the Advanced Test Reactor as well as many other programs throughout the INL. The first step in this upgrade is the updating of the gamma-ray spectrometry systems. Currently, these gamma-ray spectrometers use a standard spectroscopy amplifier and a pulser-based ADC. We have performed a series of tests to determine if a digital-signal processor-based system can replace these analog electronics, with little to no loss in performance.     

Determination of selenium in animal tissue samples using radioisotope induced X-ray fluorescence

A summary of sources of background affecting gamma-ray spectrometers and methods for eliminating each are discussed, along with practical cost/benefit ratios. Background contributed by samples generally defines practical levels for system background. The practical bottom line can be obtained for relatively modest costs. A realistic bottom line is attained in underground systems when the major contributions to the background come from cosmogenically produced⁶⁸Ge and double-beta decay of⁷⁶Ge in the detector. The true bottom line is reached with isotopically enriched detectors that eliminate these two chemically inseparable radioactive impurities. Data from isotopically enriched detectors are presented.     

Implementation of a quality system in a clinical laboratory – Evaluation of quality indicators

 The aim of this study was to evaluate the primary experience of implementing a quality system in a clinical laboratory. The second interrelated aim was to evaluate the quality and financial indicators needed for continuous measurement of quality, decision making in the laboratory management and everyday process control in analytical work. The quality process itself should be evaluated because the building up of a quality system requires a considerable amount of resources. The most effective and practical ways of using a quality system as a management tool should be found and the need for financial appraisal when the quality system is implemented is stressed. According to our study, when the effects of the quality system were evaluated, the managers of the laboratory had not considered the appropriate financial indicators. The quality indicators considered to be the best were internal quality control, external quality assessment and customer satisfaction surveys. The first benefits of the quality system evaluated by the personnel were other than the purely financial benefits, they include a more systematic and empowering approach to laboratory management, better working instructions, better knowledge of the methods and equipment, and fewer errors. The financial evaluation of a quality process in a public-owned clinical laboratory is complicated due to the fact that financial indicators are not as far developed and diverse as in industrial organisations. When starting to implement a quality system, it is important to pay attention to all measures that motivate the staff and help them benefit from the practical effects of the system. Received: 10 November 1999 / Accepted: 12 January 2000     

The SPECTRA program library: A PC based system for gamma-ray spectra analysis and INAA data reduction

A PC based system has been developed for the analysis of gamma-ray spectra and for the complete reduction of data from INAA experiments, including software to average the results from multiple lines and multiple countings and to produce a final report of analysis. Graphics algorithms may be called for the analysis of complex spectral features, to compare the data from alternate photopeaks and to evaluate detector performance during a given counting cycle. A database of results for control samples can be used to prepare quality control charts to evaluate long term precision and to search for systematic variations in data on reference samples as a function of time. The entire software library can be accessed through a user-friendly menu interface with internal help.     

New cooling methods for HPGE detectors and associated electronics

Summary Despite the on-going development of room temperature semiconductors for use as gamma-ray detectors, the only material which can provide a solution to the combined requirements of stability, high-energy resolution and high-detection efficiency (at useful energies) is still germanium (HPGe). These properties of HPGe gamma-ray detectors make them invaluable in meeting the demands of the newly emergent and increasingly important applications relating to homeland security and the interdiction of smuggled nuclear material. However, HPGe detectors require cooling to cryogenic temperatures (<120 K) to operate as gamma-ray detectors. Traditionally, this cooling has been accomplished with liquid nitrogen (LN2). The use of LN2 as a coolant is, at best, inconvenient. Maintenance, operating cost, availability at remote locations, and the hazardous nature of the material all combine to limit the practicality of a LN2-cooled device, no matter how desirable it might be from other standpoints. Mechanical methods of achieving cryogenic temperatures have existed for many years. The first mechanically-cooled HPGe systems appeared commercially in the early 1980s.¹ These systems had high cost, high power requirements, degraded system performance, were bulky in size, and unreliable. Other developments have produced prototype versions of portable (or transportable) mechanically-cooled HPGe systems. More recent advances in mechanical cooling technologies have the potential to make HPGe detectors easily adaptable to a wide variety of applications including battery-operated, truly man-portable systems for use in inspection, unattended monitoring, and Homeland Security. The major problems of mechanical coolers are degraded performance due to vibration and power consumption. The systems described here have reduced both of these to useable limits. The vibration or microphonic noise created in real-world systems is significantly reduced by optimizing the digital filter technology in the signal processing electronics associated with such detectors. Data presented here show reliability and performance results of the mechanically-cooled systems. These results show the improvements gained through the use of the optimally-matched digital filters.     

Quality control procedures for chloride and nitrate ions analysis in plant samples by ion chromatography

This paper describes useful procedures to monitor quality of chloride and nitrate ions analysis in plant samples by ion chromatography. The use of certified reference materials (CRMs) provided an efficient way to verify the accuracy of the method. Data generated by the method of analysis for chloride compared favourably with certified values. The quality system included also the systematic analysis of an internal reference sample in each batch of samples routinely analysed. The performance of the method, including extraction and measurement, over a period of 3 years was reported with control charts. The yearly variation coefficients were less than 6.5% for chloride and nitrate ions. Finally, the analytical method was evaluated through the participation of laboratory to an international proficiency testing scheme. Found results were not significantly different from published medians.     

Recent developments in semiconductor gamma-ray detectors

Summary The successful development of lithium-drifted Ge detectors in the 1960s marked the beginning of the significant use of semiconductor crystals for direct detection and spectroscopy of gamma-rays. In the 1970s, high-purity Ge became available, which enabled the production of complex detectors and multi-detector systems. In the following decades, the technology of semiconductor gamma-ray detectors continued to advance, with significant developments not only in Ge detectors but also in Si detectors and room-temperature compound-semiconductor detectors. In recent years, our group at Lawrence Berkeley National Laboratory has developed a variety of gamma-ray detectors based on these semiconductor materials. Examples include Ge strip detectors, lithium-drifted Si strip detectors, and coplanar-grid CdZnTe detectors. These advances provide new capabilities in the measurement of gamma-rays, such as the ability to perform imaging and the realization of highly compact spectroscopy systems.     

Recent and future developments in low power total reflection X-ray fluorescence spectroscopy

Today, energy-dispersive X-ray fluorescence (EDXRF) spectroscopy with low power X-ray tubes and thermoelectrically cooled detectors provide analytical performance which in the past was restricted to systems with kW power X-ray tubes and liquid nitrogen cooled Si(Li) detectors. Especially for low power TXRF spectrometers, the sensitivity could be improved by an order of one magnitude in the last 5 years. This progress was mainly based on improvements in quantum efficiency of all components and less on high power excitation sources.Recent developments caused further improvements in the analytical sensitivity as well as in the analytical performance.The introduction of a micro-focus X-ray tube increased the excitation power by a factor of 1.3. An additional improvement could be achieved by optimizing the detector window design. By optimizing the detector entrance geometry, the solid detection angle of a silicon drift detector (SDD) was increased by a factor of 1.8. In addition, the recent development of a new generation of silicon drift detectors increased the active detector area by a factor of three enhancing the peak to background ratio by a factor of two. Furthermore, the high-energy efficiency of this new detector type was significantly improved.As a result of all these improvements the detection limit for nickel could be decreased to a value of 1 pg.     

Laser-induced breakdown spectroscopy—From research to industry,new frontiers for process control

This paper presents R&D activities to explore new laser parameter ranges in pulse energy, time and space for laser-induced breakdown spectroscopy. The collinear double pulse effect, which is well studied for pulses of typically several 100 mJ energy can also be observed for laser pulses having a pulse energy two orders of magnitude lower. In this case, maximum line emission intensity occurs at interpulse separations of a few 100 ns. Temporal pulse tailoring to improve the performance of LIBS is only a first step. A comprehensive approach includes spatial pulse shaping to generate craters with predefined shape or to improve spatial averaging for the analysis of inhomogeneous samples. High performance components for LIBS systems such as spectrometers, electronics and sample stands are required to enable industrial applications. Latest developments offer wide-band single spectra acquisition with a high spectral resolution at a measuring frequency of up to 500 Hz. The next generation of multi-channel integrator electronics for Paschen–Runge spectrometers equipped with PMT detectors will further push the measuring speed to up to 5 kHz, thus opening a new area of high-speed LIBS microanalysis. Novel LIBS devices for various industrial applications presented include analysis of metallic process control samples with scale layers, on-site analysis of slag samples in secondary metallurgy, high-speed identification of Al scrap, mix-up detection of pipe fittings as well as recent work towards in-process identification of hot coils in a rolling mill.     

Achieving ultralow background in a germanium spectrometer

A germanium diode gamma-ray spectrometer has been constructed that exhibits background levels three orders of magnitude lower than conventional low-background laboratory spectrometers in the energy region around 100 keV and five orders of magnitude lower in the energy region above 3 MeV. The steps necessary to achieve this reduction are described, and the application of this technology to construction of ultralow background laboratory based germanium diode gamma-ray spectrometers is discussed.Operated for the U.S. Department of Energy by Battelle Memorial Institute under Contract DE-AC06-76RLO 1830.     

Strategies for internal quality control in antidoping analyses

Internal quality control (IQC) is one of the most important elements contributing to quality assurance in the laboratory. In this study, the strategy for the implementation of an IQC program to monitor performance of the analytical procedures used in an antidoping control laboratory is presented. Different IQC parameters have been defined according to the aim of the method (qualitative or quantitative, screening or confirmation). They are based on the analysis of control and calibration samples in each analytical batch and on the use of an internal standard in chromatographic methods. IQC parameters for chromatographic and immunological methods and the acceptance criteria used to check the quality control data obtained are described and discussed. These IQC procedures have been applied during routine antidoping analyses of more than 5000 samples per year in a laboratory accredited by the International Olympic Committee (IOC) and meeting the requirements of the quality standard ISO 17025.     

Technical Factors of Quality Management in Gamma-Ray Spectrometry of Environmental Samples

The establishment of a quality management system is the best way to comply with international requirements concerning the achievement of confident and traceable analytical results. Some important points dealing with the technical factors of quality management in gamma-ray spectrometry of environmental samples are discussed. The experience obtained from analytical procedure validation is presented. Results of the application of standardized procedures to the analysis of ALMERA intercomparison samples, as well as the outcome of the utilization of certified reference materials for the quality control of measurement are presented. In fact, the implantation of simple technical principles reports reliable results and allows to elevate the quality of the measurements at a cost relatively low according to the real possibilities of the small laboratories, even in developing countries.     

Radon Mapping of Soils in St. Elizabeth, Jamaica

Soil gas measurements of radon were made in St. Elizabeth, Jamaica using nuclear track etch detectors. The results were compared to gamma-ray spectroscopy measurements made in the laboratory on soil samples collected at the radon measurement sites. An assessment of the degree of disequilibrium of uranium and thorium was also made by comparison with neutron activation analysis, delayed neutron counting and equivalent uranium and thorium measurements. The results to date for equivalent uranium and radon show a strong correlation and indicate the possibility of soil radon mapping in Jamaica using gamma-ray spectroscopy. Three anomalous sites have been identified.     

Application of epithermal neutron activation in multielement analysis of silicate rocks employing both coaxial Ge(Li) and low energy photon detector systems

The instrumental activation analysis of silicate rocks using epithermal neutrons has been studied using both high resolution coaxial Ge(Li) detectors and low energy photon detectors, and applied to the determination of 23 elements in eight new U.S.G.S. standard rocks. The analytical use X-ray peaks associated with electron capture or internal conversion processes has been evaluated. Of 28 elements which can be considered to be determinable by instrumental means, the epithermal activation approach is capable of giving improved sensitivity and precision in 16 cases, over the normal INAA procedure. In eleven cases the use of the low energy photon detector is thought to show advantages over convertional coaxial Ge(Li) spectroscopy.     

Evolution of an open-access quantitative bioanalytical mass spectrometry service in a drug discovery environment

Increased demand for assays for compounds at the early stages of drug discovery within the pharmaceutical industry has led to the need for open-access mass spectrometry systems for performing quantitative analysis in a variety of biological matrices. The open-access mass spectrometers described here are LC/MS/MS systems operated in 'multiple reaction monitoring' (MRM) mode to obtain the sensitivity and specificity required to quantitate low levels of pharmaceutical compounds in an excess of biological matrix. Instigation of these open-access systems has resulted in mass spectrometers becoming the detectors of choice for non-expert users, drastically reducing analytical method development time and allowing drug discovery scientists to concentrate on their core expertise of pharmacokinetics and drug metabolism. Setting up an open-access facility that effectively allows a user with minimal mass spectral knowledge to exploit the MS/MS capability of triple quadrupole mass spectrometers presents a significantly different challenge from setting up qualitative single stage mass spectrometry systems. Evolution of quantitative open access mass spectrometry within a pharmaceutical drug metabolism and pharmacokinetics group, from its beginnings as a single generic system to a series of specialist fully integrated walk-up facilities, is described.     

Influence of a quality system complying with the requirements of ISO/IEC 17025 standard on the management of a gamma-ray spectrometry laboratory

The motives for and the implementation of a quality system complying with the requirements of the ISO/IEC 17025 standard in a gamma-ray spectrometry laboratory are briefly described, as well as its influence on the laboratory's work and output. The use of the quality system as a tool for managing and controlling the state of the laboratory is described. Two examples of control and improvement of the laboratory's performance are given.     

Determination of the 209Bi(n,γ) capture cross section at a cold neutron beam

Summary The total capture cross section of ²⁰⁹Bi was determined at the cold neutron beam PGAA-NIPS facilities at the Budapest Neutron Centre. The measurements were performed using a coaxial HPGe detector with Compton suppression. The total and partial gamma-ray production cross sections were deduced relative to the ¹⁴N(n,γ) partial gamma-ray production cross section. By using a bismuth nitrate stoichiometric compound as the sample, we excluded various systematic uncertainties. The total capture cross section is in very good agreement with the compilation of Mughaghab, but is slightly lower than the most recent value determined at the high flux reactor of the ILL in Grenoble, France. We also performed measurements using a 0.5 mm thin Bi metal disc. The relative intensities determined from the Bi disc and the compound samples are in good agreement.