Anticosmic-shielded ultralow-background germanium detector systems for analysis of bulk environmental samples

A low-level gamma-ray counting system has been developed which reduces system background, relative to other typical low-background systems, by a factor of ten in the energy region below one MeV, and by as much as a factor of forty at higher energies. This germanium-diode gamma-ray spectrometer was constructed for a modest investment above that required for a conventional germanium detector. The techniques involved use: (1) materials of known radiopurity to surround the diode, (2) an active external anticosmic shield to reduce the background continuum due to interactions of cosmic particles with the detector and passive lead shielding, and (3) nitrogen exhausted from the cryogenic dewar to minimize the introduction of ubiquitous radon decay nuclei into the sample counting chamber. A novel method for handling samples prior to counting is presented. Also; some of the difficulties encountered in calibrating a system intended for bulk samples are discussed.Operated for the U.S. Department of Energy by Battelle Memorial Institute under Contract DE-AC06-76RLO 1830.     

Next-generation germanium spectrometer background reduction techniques at 2 Me

Summary The Majorana project, a next-generation ⁷⁶Ge neutrinoless double-beta decay experiment being undertaken by a large international collaboration, has the goal of measuring the neutrinoless double-beta decay rate by observing monochromatic events at 2039 keV in 500 kg of isotopically enriched ⁷⁶Ge gamma-ray spectrometers. In order to achieve the desired sensitivity limit, the background in the 2037-2041 keV region must be reduced to <1 event per year in the entire germanium array. The effects of various background reduction techniques, and the combination thereof, to produce a huge ⁷⁶Ge spectrometer array with virtually zero background are discussed.     

Prompt Gamma Neutron Activation Analysis of 316-L Stainless Steel

Prompt gamma-rays from thermal neutron capture reaction have been used to measure the concentrations of the main constituents namely Fe, Ni and Cr in 316-L stainless steel using recently established prompt gamma neutron activation analysis (PGNAA) facility at Pakistan Institute of Nuclear Science and Technology (PINSTECH). High resolution, high purity germanium detector with 40% relative efficiency was employed for the gamma-ray spectroscopy of the samples. The interference-free full energy gamma-ray peaks of the elements of interests were selected in the high energy low background region (5.0–9.0 MeV). The efficiency calibration of the detector was performed using ultra pure standards of chromium and chlorine obtained respectively from Merck and Alpha Inorganics. This paper describes, in addition, the salient features as well as the background of establishing PGNAA facility at the Institute.     

The neutron activation analysis laboratory at the Ecole polytechnique de Montreal

The SLOWPOKE reactor at the Ecole Polytechnique de Montréal has been used for neutron activation analysis since 1976. The reproducible neutron flux in the five irradiation sites may be set to values between 10¹⁰ and 10¹² cm^–2s^–1. Associated equipment includes versatile pneumatic sample transfer systems and three germanium gamma-ray spectrometers with mechanical sample changers. The laboratory is used by researchers from several universities and by a variety of industries.     

Methods and software for predicting germanium detector absolute full-energy peak efficiencies

High-purity germanium (HPGe) and lithium drifted germanium (Ge(Li)) detectors have been the detector of choice for high resolution gamma-ray spectroscopy for many years. This is primarily due to the superior energy resolution that germanium detectors present over other gamma-ray detectors. In order to perform quantitative analyses with germanium detectors, such as activity determination or nuclide identification, one must know the absolute full-energy peak efficiency at the desired gamma-ray energy. Many different methods and computer codes have been developed throughout history in an effort to predict these efficiencies using minimal or no experimental observations. A review of these methods and the computer codes that utilize them is presented.     

A study of the indium and germanium photopeaks in the background spectra of Ge spectrometers with a passive shield

Cosmic ray neutron interactions with indium, used as electrical contact within a Ge diode, the diode itself and the surrounding materials can give rise to a large number of photopeaks in the 50 to 1300 keV region of background spectra of Ge spectrometers with a passive shield. The nuclear processes and decays involved in the production of these photopeaks are discussed. These cosmic ray produced photopeaks are compared with those due to primordial radionuclides. Some useful information can be drawn from these measurements on the contribution of the cosmic rays on the background of Ge detectors with a passive shield.     

Performance and robustness of a multi-user, multi-spectrometer system for INAA

The laboratory for instrumental neutron activation analysis at the Reactor Institute Delft, Delft University of Technology uses a network of 3 gamma-ray spectrometers with well-type detectors and 2 gamma-ray spectrometers with coaxial detectors, all equipped with modern sample changers, as well as 2 spectrometers with coaxial detectors at the two fast rabbit systems. A wide variety of samples is processed through the system, all at specific optimized (and thus different) analytical protocols, and using different combination of the spectrometer systems. The gamma-ray spectra are analyzed by several qualified operators. The laboratory therefore needs to anticipate on the occurrence of random and systematic inconsistencies in the results (such as bias, non-linearity or wrong assignments due to spectral interferences) resulting from differences in operator performance, selection of analytical protocol and experimental conditions. This has been accomplished by taking advantage of the systematic processing of internal quality control samples such as certified reference materials and blanks in each test run. The data from these internal quality control analyses have been stored in a databank since 1991, and are now used to assess the various method performance indicators as indicators for the method’s robustness.     

Ultrahigh energy resolution gamma-ray spectrometers for precision measurements of uranium enrichment

Superconducting gamma-ray detectors offer an order of magnitude higher energy resolution than conventional high-purity germanium detectors. This can significantly increase the precision of non-destructive isotope analysis for nuclear samples where line overlap affects the errors of the measurement. We have developed gamma-detectors based on superconducting molybdenum-copper sensors and bulk tin absorbers for nuclear science and national security applications. They have, depending on design, an energy resolution between ∼50 and ∼150 eV FWHM at ∼100 keV. Here, we apply this detector technology to the measurement of uranium isotope ratios, and discuss the trade-offs between energy resolution and quantum efficiency involved in detector design.     

Comparison of background gamma-ray spectra between Los Alamos, New Mexico and Austin, Texas

Background counts in gamma-ray spectrometry are caused by a variety of sources. Among these are naturally occurring radioactive materials (NORM) in the environment, interactions from cosmic radiation, and contamination within the laboratory. High-purity germanium detectors were used to acquire long background spectra in Los Alamos, NM (elevation ~7,300 feet) and Austin, TX (elevation ~500 feet). This difference in elevation has a sizeable effect on background spectra due to cosmic interactions, such as (n,n′) and (n,γ). Los Alamos also has a fairly high NORM concentration in the soil relative to Austin, and this gives way to various spectral interferences. When analyzing nuclear forensics samples, these background sources can have non-trivial effects on detection limits of low-level fission products. By accurately determining the influence that elevation and environment have on background spectra, interferences within various laboratory environments can be more accurately characterized.     

Recent developments of prompt gamma activation analysis at Budapest

The PGAA facility at the Budapest Research Reactor has been continually upgraded and developed since its start-up in 1996, as a result of which its performance has improved considerably. The installation of the cold neutron source, the partial change to supermirror neutron guides and their realignment increased the flux by almost two orders of magnitude. The data acquisition has been modernized as well; digital spectrometers were tested and implemented in novel forms of gamma-ray spectrum collection. This year a higher-efficiency HPGe detector and a new data acquisition module were put into operation. Most recently all the neutron guides were changed to supermirror-coated ones to further increase the neutron flux. The improved evaluation software makes possible a more reliable elemental analysis of the samples. In this progress report these developments are critically reviewed. The characteristics of the latest system are also described. It is the first time that a set of new partial gamma-ray production cross sections are presented, which are based on the new intensity values of ¹⁴N(n,γ)¹⁵N calibration standard.     

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.     

A preliminary screening technique for selected metals at waste sites

Fast neutron activation analysis (FNAA) was investigated as a possible on-site preliminary screening technique for metal contamination of soil. Two metals, Cu and Zn, were used in a laboratory setting to evaluate the possibility of detecting metal contamination of soil at or below the maximum permissible metal concentration in soil. Varying quantities of compounds of the selected metals were mixed into a prepared soil column for analysis of signal intensity as a function of concentration in the soil. Experiments were conducted with a sealed tube neutron generator and a germanium gamma-ray detector. Both metals produced signal levels distinguishable from background soil concentrations at the maximum permissible level.     

GAMANAL-PC: A program for gamma-ray spectrum analysis using a microcomputer

The gamma-ray spectrum analysis program, GAMANAL, has been modifed to operate on a microcomputer. The program uses an algorithm involving a Gaussian and a tailing term for fitting and resolving peaks obtained from spectrometers using germanium semiconductor detectors. Gamma-ray energies, intensities and absolute photon emission rates can be determined. A graphical output showing the original and fitted data can also be obtained. The results generated by the program are stored on disk as ASCII files for futher analysis. This allows the use of other computer programs and languages in tasks such as decay curve analysis, radionuclide activity measurements and neutron activation analysis.     

Advantages of low-background liquid scintillation alpha-spectrometry and pulse shape analysis in measuring222Rn, uranium and226Ra in groundwater samples

Liquid scintillation counting (LSC) and pulse shape analysis (PSA) was used in measuring radon and gross alpha- and beta-activities in groundwater. We used conventional LSC counters for the measurement of radon in water, but low-background LSC spectrometers for the gross activity measurements. The lower limit of detection (LLD) for radon in water is 0.6 Bq/l for a 60 min count with a conventional counter, but 0.1 or 0.2 Bq/l, with the two types of low-background LSC spectrometers equipped with a pulse shape analyser (PSA). The gross alpha and beta activity measurements are made using a simple sample preparation method, PSA of a low background LSC and spectrum analysis. The LLD recorded for gross alpha and beta with the two spectrometers are 0.02 and 0.03 Bq/l and 0.2 and 0.4 Bq/l, respectively, for a 180 minutes count and a 38 ml sample volume. The method also enable the calculation of the U and²²⁶Ra contents in water and indicates the presence of some other long-lived radionuclides (²¹⁰Pb,²²⁸Ra or⁴⁰K). The LLD for U recorded with both spectrometers is 0.02 Bq^–1 and for²²⁶Ra 0.01 Bq·1^–1. The LLDs attained by this LSC method are two orders of magnitude lower than the maximum permissible concentrations set for U and²²⁶Ra.     

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.     

Balloon-borne near-infrared diode laser spectroscopy for in situ measurements of atmospheric CH4 and H2O

Absorption spectroscopy with near-infrared telecommunication laser diodes is a very convenient technique to measure in situ methane and water vapor in both the troposphere and the lower stratosphere (LS) and thereby to address many topics in the science of the atmosphere. This technique offers a high temporal resolution that ranges from 10 ms to 1 s, a precision error in the concentration retrieval of within a few percents and a dynamic range for the measurements of four orders of magnitude. A balloon-borne near-infrared diode laser spectrometer is described that provides simultaneous in situ methane (in the 1.65-microm region) and water vapor (in the 1.39-microm region) measurements at 1 s intervals. Tropospheric and stratospheric vertical concentration profiles of methane and water vapor are reported.     

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.     

Evaluation of digital pulse processing-based gamma-ray spectroscopy under neutron activation analysis conditions

Digital signal processors are now available commercially for incorporation into high resolution gamma-ray spectroscopy systems. In this work, we have compared throughput, peak resolution and peak stability found in two Canberra 2060 Digital Spectrum Processors with a conventional analog processing setup in our laboratory. We have made the comparisons for five separate high purity germanium detectors which provide a range in detector size and construction. In addition, the range of input count rates chosen for study reflect those likely to be encountered in NAA. Our initial results indicate the performance to be detector specific and highly dependent on DSP setup parameters.     

Background of low-level gamma-ray spectrometer due to the atmospheric 220Rn and 222Rn

In connection with low-level gamma-ray counting of natural samples, background due to 220Rn- and 222Rn-daughters was monitored. The results obtained for 4 months showed that the background gamma-ray from 222Rn-daughters was more variable than that of 220Rn-daughters. An efficient air-conditioning was helpful to keep the background stable. It was practically equivalent to the use of N2-gas. Radiometric data for dust samples filtered from the laboratory air suggested that Rn-daughters tended to be removed by air-conditioning.     

Determination of alcohol content in beverages using short-wave near-infrared spectroscopy and temperature correction by transfer calibration procedures

This paper reports the utilization of short-wave near-infrared (SW-NIR) transmission spectroscopy for rapid and conclusive analysis of alcoholic content (% v/v) in beverages. This spectral region is interesting because common visible diode array spectrometers can be utilized, reducing time and costs in comparison with traditional near-infrared or mid-infrared instruments. A correction of external temperature influence is necessary, and for this purposes two calibration transfer procedures were compared: piecewise direct standardization (PDS) and orthogonal signal correction (OSC). The RMSEP found for the alcoholic content model at 20 °C was 0.13% v/v and, after application of transfer calibration procedures at other temperatures (15, 25, 30 and 35 °C) using the model built at 20 °C, errors of the same order of magnitude were obtained.