A field-deployable, aircraft-mounted sensor for the environmental survey of radionuclides

The Environmental Radionuclide Sensor System (ERSS)³ is an extremely sensitive sensor, which has been cooperatively developed by Pacific Northwest National Laboratory (PNNL) and Special Technologies Laboratory (STL) for environmental surveys of radionuclides. The ERSS sensors fit in an airborne pod and include twenty High-Purity Germanium (HPGe) detectors for the high-resolution measurement of gamma-ray emitting radionuclides, twenty-four³He detectors for possible neutron measurements, and two video cameras for visual correlation. These acrial HPGe sensors provide much better gamma-ray energy resolution than can be obtained with NaI(TI) detectors. The associated electronics fit into three racks. The system can be powered by the 28 V DC electrical supply of typical aircraft or 120 V AC. The data acquisition hardware is controlled by customized software and a real-time display is provided. Each gamma-ray event is time stamped and stored for later analysis. This paper will present the physical design, discuss the software used to control the system, and provide some examples of its use.     

Compton suppression system at Penn State Radiation Science and Engineering Center

A Compton suppression system is used to reduce the contribution of scattered gamma-rays that originate within the HPGe detector to the gamma-ray spectrum. The HPGe detector is surrounded by an assembly of guard detectors, usually NaI(T1). The HPGe and NaI(T1) detectors are operated in anti-coincidence mode. The NaI(T1) guard detector detects the photons that Compton scatter within, and subsequently escape from the HPGe detector. Since these photons are correlated with the partial energy deposition within the detector, much of the resulting Compton continuum can be subtracted from the spectrum reducing the unwanted background in gamma-ray spectra. A commercially available Compton suppression spectrometer (CSS) was purchased from Canberra Industries and tested at the Radiation Science and Engineering Center at Penn State University. The PSU-CSS includes a reverse bias HPGe detector, four annulus NaI(T1) detectors, a NaI(T1) plug detector, detector shields, data acquisition electronics, and a data processing computer. The HPGe detector is n-type with 54% relative efficiency. The guard detectors form an annulus with 9-inch diameter and 9-inch height, and have a plug detector that goes into/out of the annulus with the help of a special lift apparatus to raise/lower. The detector assembly is placed in a shielding cave. State-of-the-art electronics and software are used. The system was tested using standard sources, neutron activated NIST SRM sample and Dendrochronologically Dated Tree Ring samples. The PSU-CSS dramatically improved the peak-to-Compton ratio, up to 1000:1 for the ¹³⁷Cs source.     

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.     

A software package using a mesh-grid method for simulating HPGe detector efficiencies

Traditional ways of determining the absolute full-energy peak efficiencies of high-purity germanium (HPGe) detectors are often time consuming, cost prohibitive, or not feasible. A software package, KMESS (Kevin’s Mesh Efficiency Simulator Software), was developed to assist in predicting these efficiencies. It uses a semi-empirical mesh-grid method and works for arbitrary source shapes and counting geometries. The model assumes that any gamma-ray source shape can be treated as a large enough collection of point sources. The code is readily adaptable, has a web-based graphical front-end, and could easily be coupled to a 3D scanner. As will be shown, this software can estimate absolute full-energy peak efficiencies with good accuracy in reasonable computation times. It has applications to the field of gamma-ray spectroscopy because it is a quick and accurate way to assist in performing quantitative analyses using HPGe detectors.     

Monte Carlo and experimental efficiency calibration of gamma-spectrometers for non-destructive analysis of large volume samples of irregular shapes

A comparison of efficiency calibration of a HPGe gamma-ray spectrometer applied for non-destructive analysis of gamma-ray emitters in large volume samples of irregular shape is presented. The detector efficiency calibration was carried out during the analysis of cosmogenic radionuclides (⁶⁰Co, ⁵⁴Mn, ²²Na and ²⁶Al) in fragments of the Ko?ice meteorite. Fourteen meteorite fragments were available for the analysis with masses from 27 to 2,163 g. A reasonable agreement in the estimation of the HPGe detector efficiency was obtained using the Monte Carlo simulation GEANT 3 code, and the experimental calibration using radioactive standards mixed with iron–silica–copper powder housed in mock-ups of similar shapes as the original samples. The differences in the efficiency estimation obtained by both methods were within 10 %. It is recommended that the Monte Carlo simulation of the detector efficiency can be applied in routine analysis of gamma-ray emitters in large volume samples of regular or irregular shapes.     

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.     

Low-level single and coincidence gamma-ray spectrometry

Analyses of anthropogenic and natural gamma-ray emitters in the environment require high sensitive detector systems operating in coincidence-anticoincidence modes. Thanks to an excellent energy resolution and a high efficiency, large volume HPGe detectors have been widely used in low-level gamma-ray spectrometry. In the present paper we discuss the characteristics of single and coincidence (HPGe-NaI(Tl)) arrangements suitable for analysis of environmental samples containing cascade gamma-ray emitters (e.g., ⁶⁰Co), positron emitters (e.g., ²²Na) and single gamma-ray emitters (e.g., ¹³⁷Cs). The detectors were placed in a large volume shields consisting of iron, lead and copper layers. The reduction of background for the single gamma-ray spectrometer is between 60 and 250, depending on the gamma-ray energy. As an improvement of the apparatus, low detection limits for analysis of ¹³⁷Cs (0.3 Bq·kg⁻¹) and ⁶⁰Co (0.1 Bq·kg⁻¹) in environmental samples, respectively, have been obtained.     

Development of a multidimensional gamma-spectrometer

A high-sensitivity multidimensional gamma-spectrometer is being developed within the shallow underground laboratory at Pacific Northwest National Laboratory (PNNL, USA). The system consists of two broad energy germanium detectors, inside a low-background shield, fitted with a cosmic veto system. The detector has advanced functionality, including operation in single or combined detector mode, with reductions in the cosmic background of 49.6% and Compton suppression of 6.5%. For selected radionuclides this provides increased peak identification, reductions in uncertainty of 27.6% and MDA improvements of 52.7%. The design uses commercially off-the-shelf components to provide a powerful solution for low-level nuclear measurements.     

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.     

Calculation of peak-to-total ratios for high purity germanium detectors using Monte-Carlo modeling

Summary In order to estimate by calculation the magnitude of the true coincidence summing losses that may be affecting the observed gamma-ray spectrum of a given nuclide, measured using a spectrometer, knowledge of the total detection efficiencies at the gamma-ray energies within the cascades is essential. The total efficiency can be determined from the full energy peak efficiency, provided the peak-to-total ratio is known. For a given high purity germanium (HPGe) detector, one can establish an intrinsic peak-to-total (P/T) efficiency curve using a set of measurements performed with “single” (ideally monoenergetic) gamma-emitting nuclides (e.g., ²⁴¹Am, ¹⁰⁹Cd, ⁵⁷Co, ¹¹³Sn, ¹³⁷Cs, ⁶⁵Zn). Some of these nuclides are short lived and so have to be replaced periodically. Moreover, the presence of low energy gamma-rays and X-rays in most of the decay schemes complicate the empirical determination of the P/T ratios. This problem is especially severe if measurements are made using HPGe detectors that have a very thin dead layer. The problems posed by low energy gamma-rays and X-rays can be avoided by using absorbers, but then one has to be careful not to perturb the intrinsic value of the P/T ratio being sought. This paper addresses these problems. Measurement related limitations are avoided if one can use a computational technique instead. In the work presented here, the feasibility of using a Monte-Carlo based technique to determine the P/T ratios at a wide range of energies (60 keV to 2000 keV) is explored. The Monte-Carlo code MCNP (version 4B) is used to simulate gamma-ray spectra from various nuclides. Measured P/T ratios are compared to calculated ratios for several HPGe detectors to demonstrate the generality of the approach. Reasons for observed disagreement between the two are discussed.     

Pulse tube refrigeration for detectors

High purity germanium (HPGe) gamma-ray detectors are used for nondestructive assay. Liquid nitrogen (LN₂), a cryogen, is commonly used to cool these detectors. Cryogen use is associated with several health risks and operational problems. This has prompted the development of cryogen-free refrigeration. A new generation of commercial pulse tube refrigerator (PTR) has been developed during the last decade. A unique feature of the PTR is the absence of cold moving parts. This significantly reduces the generated noise and vibration. In the following report, LN₂, a modified Joule–Thompson cooler, and a PTR unit are examined and their cooling effectiveness with HPGe gamma-ray detectors compared. Overall, PTR is an engineering equivalent to LN₂ and modified Joule–Thompson cooler systems used in gamma spectroscopy and eliminate the health and physical hazards associated with LN₂ systems without adding hazards.     

Assessment of the suitability of Monte Carlo simulation for activity measurements of extended sources

Monte Carlo simulations can be a powerful tool in calibrating high-resolution gamma-ray spectrometry based on high pure germanium (HPGe) detectors. The purpose of this work is to examine the applicability of Monte Carlo simulations for the computation of the efficiency transfer in various measurement geometries on the basis of the detected efficiency for point source geometry. For this, GEANT4 code was applied for the computation of the detection efficiency for incident gamma energy of radionuclide placed at different distances from HPGe detector from 50 to 2,000 keV in addition for volume sources of different compositions and densities. The experimental efficiency curves were compared with the prediction of the GEANT4 code. Efficiency is computed at discrete values of point and volume sources in different distances to derive new efficiencies values for other distances.     

A dual purpose Compton suppression spectrometer

A gamma-ray spectrometer with a passive and an active shield is described. It consists of a HPGe coaxial detector of 42% efficiency and 4 NaI(Tl) detectors. The energy output pulses of the Ge detector are delivered into the 3 spectrometry chains giving the normal, anti- and coincidence spectra. From the spectra of a number of ¹³⁷Cs and ⁶⁰Co sources a Compton suppression factor, SF and a Compton reduction factor, RF, as the parameters characterizing the system performance, were calculated as a function of energy and source activity and compared with those given in literature. The natural background is reduced about 8 times in the anticoincidence mode of operation, compared to the normal spectrum which results in decreasing the detection limits for non-coincident gamma-rays up to a factor of 3. In the presence of other gamma-ray activities, in the range from 5 to 11 kBq, non- and coincident, the detection limits can be decreased for some nuclides by a factor of 3 to 5.7.     

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.     

Low-level radioactive waste measurement comparisons of three gamma-ray counting systems

Three different gamma-ray counting systems constructed by 1–3 HPGe detectors were used in this study to compare their system performance. One measurement scheme involved positioning a single HPGe detector on a movable cart with a 90° collimation angle to the observed item. The other two waste assay systems were configured with two or three HPGe detectors towards the sample drums, while the three-HPGe-detector counting system was in a shielded counter cavity. The measurement consistency of 38 low-level waste drums, system operating costs and acquisition times to achieve the same MDA for these counting systems were compared and discussed in this study.     

A neutron induced prompt gamma-ray spectroscopy system using a 252Cf neutron source for quantitative analysis of aqueous samples

A neutron induced prompt γ -ray spectrometry (NIPS) facility has been developed at the Nuclear Chemistry Research Division, of the Korea Atomic Energy Research Institute (KAERI) with the aim of analyzing the major components of various elements in aqueous samples. The facility is equipped with a ²⁵²Cf neutron source and a γ-γ coincidence setup with two n-type coaxial HPGe detectors based on NIM spectrometric modules in association with data acquisition and spectral analysis systems. The development of the system, its set-up and the calibration of detection efficiency up to 8 MeV using a set of radionuclides and the (n,γ) reactions of chlorine are described in the paper. This revised version was published online in July 2006 with corrections to the Cover Date.     

Monitoring of radioactivity in NW Irish Sea water using a stationary underwater gamma-ray spectrometer with satellite data transmission

Summary An underground laboratory for low-level gamma- and beta-spectrometry has been constructed at IAEA-MEL, Monaco, for the analysis of environmental radionuclides. The laboratory is situated at a depth of 35 m water equivalent underground and equipped with 4, large volume HPGe detectors placed in a common lead shield with anti-cosmic plastic scintillator shielding. There is also an anti-Compton gamma-spectrometer, comprized of an HPGe detector and NaI(Tl) shielding, and finally, a Quantulus liquid scintillation spectrometer. The performance of the gamma-spectrometers with different shielding settings/adjustments are discussed, as well as their possible applications in the analysis of natural and anthropogenic radionuclides in the marine environment.     

IAEA-MEL’s underground counting laboratory (CAVE) for the analysis of radionuclides in the environment at very low-levels

Summary An underground laboratory for low-level gamma- and beta-spectrometry has been constructed at IAEA-MEL, Monaco, for the analysis of environmental radionuclides. The laboratory is situated at a depth of 35 m water equivalent underground and equipped with 4, large volume HPGe detectors placed in a common lead shield with anti-cosmic plastic scintillator shielding. There is also an anti-Compton gamma-spectrometer, comprized of an HPGe detector and NaI(Tl) shielding, and finally, a Quantulus liquid scintillation spectrometer. The performance of the gamma-spectrometers with different shielding settings/adjustments are discussed, as well as their possible applications in the analysis of natural and anthropogenic radionuclides in the marine environment.     

Comparison between HPGe and CdZnTe detector for the correlation between calculated radioactivity and measured dose using an activated concrete sample

An activated concrete sample was counted at different source to detector distances with CdZnTe and HPGe detectors. The experimental count rates for different radionuclides were converted to dose rate using Monte Carlo code and compared with the Measured dose rates obtained using digital survey meter. The results agreed well for both the detectors. This indicates that CdZnTe detector having a better portability but poorer resolution than HPGe detector can be effectively used for online monitoring of radioactivity as well as dose rate calculations.     

Direct and precise determination of environmental radionuclides in solid materials using a modified Marinelli beaker and a HPGe detector.

A simple but precise detection method was studied for the determination of natural radionuclides using a conventional HPGe detector. A new aluminium beaker instead of a plastic Marinelli beaker was constructed and examined to reach radioactive equilibrium conditions between radon and its daughter elements without the escape of gaseous radon. Using this beaker fifteen natural radionuclides from three natural decay series could be determined by direct gamma-ray measurement and sixteen radionuclides could be determined indirectly after radioactive equilibrium had been reached. Analytical results from ground water were compared with those from conventional alpha spectroscopy and the results agreed well within 12% difference. Nitrogen gas purge was used to replace the surrounding air of the detector to obtain a stable background and reducing the interference of radon daughter nuclides in the atmosphere. The use of nitrogen purging and the aluminium Marinelli beaker results in an approximately tenfold increase of sensitivity and a decrease of the detection limit of 226Ra to about 0.74 Bq kg(-1) in soil samples.