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.     

Performance of a portable, electromechanically-cooled HPGe detector for site characterization

Characterization is a first step to site cleanup or decommissioning of a disused nuclear facility. Good knowledge of the inventory of nuclides present, both type and location, is important in the design of an effective plan of remediation. Several systems based on HPGe detectors have been developed, both commercially and at laboratories, and are already in use for this purpose. Their use is somewhat complicated by the need for cryogenic cooling of the HPGe detector. Handling of liquid nitrogen in field situations is always difficult. Recent developments in low-power electromechanical cooling for HPGe detectors have made possible the construction of low weight, portable HPGe spectrometers with sufficient efficiency to perform the needed measurements in reasonable count times, without the need for liquid nitrogen. A mobile system was modified to use a battery-powered, Sterling-engine cooler on a nominal 40% relative efficiency detector. This system was characterized for efficiency and uniformity of response. The baseline spectra were analyzed using the DOE EML 1-meter methods to obtain representative MDA values for several nuclides of interest and typical counting times.     

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.     

Monte Carlo generated spectra for QA/QC of automated NAA routine

A quality check for an automated system of analyzing large sets of neutron activated samples has been developed. Activated samples are counted with an HPGe detector, in conjunction with an automated sample changer and spectral analysis tools, controlled by the Canberra GENIE 2K and REXX software. After each sample is acquired and analyzed, a Microsoft Visual Basic program imports the results into a template Microsoft Excel file where the final concentrations, uncertainties, and detection limits are determined. Standard reference materials are included in each set of 40 samples as a standard quality assurance/quality control (QA/QC) test. A select group of sample spectra are also visually reviewed to check the peak fitting routines. A reference spectrum was generated in MCNP 4c2 using an F8, pulse-height, tally with a detector model of the actual detector used in counting. The detector model matches the detector resolution, energy calibration, and counting geometry. The generated spectrum also contained a radioisotope matrix that was similar to what was expected in the samples. This spectrum can then be put through the automated system and analyzed along with the other samples. The automated results are then compared to expected results for QA/QC assurance.     

Low-level gamma-ray spectrometry for environmental samples

Low-level gamma-ray spectrometry with large volume HPGe detectors has been widely used in analysis of environmental radionuclides. The reasons are excellent energy resolution and high efficiency that permits selective and non-destructive analyses of several radionuclides in composite samples. Although the most effective way of increasing the sensitivity of a gamma-ray spectrometer is to increase counting efficiency and the amount of the sample, very often the only possible way is to decrease the detector’s background. The typical background components of a low-level HPGe detector, not situated deep underground, are cosmic radiation (cosmic muons, neutrons and activation products), radioactivity of construction materials, radon and its progenies. A review of Monte Carlo simulations of background components of HPGe detectors, and their characteristics in coincidence and anti-Compton mode of operation are presented and discussed.     

Determination of some elements by epithermal neutron activation analysis for the Arctic aerosol

Summary We have determined nineteen trace elements in 685 aerosol filter samples collected during 1964-1978 in northern Finland by the Finnish Meteorological Institute. In this paper we present some procedures and results for very short (~25 s), short (~3-54 min), and medium (12-35 h) lived isotopes as determined by epithermal NAA in conjunction with and without Compton suppression. Elements with a I_γ/σthratio are favorable to be determined by epithermal NAA. Silver was determined by a one minute epithermal irradiation because of a very short ¹¹⁰Ag half-life. Antimony, arsenic, cobalt, bromine, indium, iodine, potassium, silicon, tin, tungsten, and zinc were determined by a ten minute epithermal irradiation. For silver determination, samples were counted without transferring the filter from the irradiated vial, however, for ten minute irradiation all samples were transferred to a non-irradiated vial and counted both in the normal and Compton mode by the HPGe gamma-spectrometry system with a decay time of about 10 minutes and counting time of 15 minutes. Each day a maximum of 16 samples were irradiated and immediately following the short counting, these samples were loaded into an automatic sample changer in sequence of irradiation and counted for an hour in both normal and Compton modes. This has proven to be an extremely cost effective measure thus reducing the need to employ long-lived NAA to analyze other elements such as Ag, Co, Sn and Zn and Ag for air pollution source receptor modeling.     

An automatic sample changer for alpha spectroscopy with a surface barrier detector

Semiconductor particle detectors are ideal for alpha spectroscopy due to their compact size, low noise, and high resolution. This paper describes the construction and testing of an automatic sample changer for use with such a detector. The changer was constructed from locally available services and materials. It holds up to 24 samples of alpha emitting material deposited on 22 mm stainless steel counting planchets. The vacuum chamber can be evacuated to less than 10 μm mercury in 10 to 15 minutes. Once the chamber has been evacuated and detector bias has been applied, any sample in the chamber may be selected for analysis, either automatically or manually. Continuous automatic analysis of up to 24 samples is possible. Variation in efficiency from position to position was found to be 3.25% at the detector-sample spacing of 4.8 mm, and 2.31% at 27 mm. Shielding between the adjacent samples not under analysis and the detector was acceptable. Published with the approval of the Director of the Arkansas Agric. Exp. Stn., Fayetteville. This project was supported in part by grants from ERDA and Arkansas Power and Light Co. and is gratefully acknowledged. Received June 18, 1979. Use of trade name does not imply endorsement or guarantee of that product to the exclusion of other products of similar nature.     

Chernobyl fallout measurements in some Mediterranean biotas

The radioactivity of various terrestrial vegetation leaves characteristic of Mediterrenean countries has been measured after the Chernobyl accident. In addition, we paid particular attention to lichens and seaweed which are considered as bioindicators of radioactive contamination. The measurements were performed by non-destructive way using both coaxial and planar HPGe detectors. For odd mass radionuclides having low energy lines, such as¹²⁵Sb or¹⁴¹Ce the sensitivity of the planar HPGe detector is better than the coaxial detector. The concentration of long lived fission nuclides remaining three months after the accident were found to be enhanced in needle form leaves and in lichens. The seaweed Sphaerococcus exhibits a strong specific activity for iodine and ruthenium and poor concentration for cesium nuclides. The activity ratios of different isotopes of the same element, measured in vegetation samples agree well with the values found by other authors in airborne aerosols. The activation nuclide¹¹⁰Ag^m is found in all samples with the same ratio¹¹⁰Ag^m/¹³⁷Cs=/1.0±0.2/×10^–2, as in the soil deposition.     

{\rtf1\ansi\ansicpg1250\deff0\deflang1038\deflangfe1038\deftab708{\fonttbl{\f0\froman\fprq2\fcharset238{\*\fname Times New Roman;}Times New Roman CE;}} \viewkind4\uc1\pard\f0\fs24 Efficiency of germanium detectors as a function of energy and incident geometry: Comparison of measurements and calculations \par }

Summary {\rtf1\ansi\ansicpg1250\deff0\deflang1038\deflangfe1038\deftab708{\fonttbl{\f0\froman\fprq2\fcharset238{\*\fname Times New Roman;}Times New Roman CE;}} \viewkind4\uc1\pard\f0\fs24 The use of HPGe detectors in counting situations where the sample is not easily reproduced has increased the use of models to determine the counting efficiency for the specific geometry. The accuracy of these simulations of the germanium detector response relies on detailed knowledge of the performance of the detector. Several different types of detectors were measured at different energies using a pencil beam of gamma-rays. These measurements showed that the dead layer was not uniform from detector to detector. This and the construction details were used to calculate the efficiency for several detectors. \par }     

Optimization of HANARO cold neutron induced prompt gamma activation analysis system by using Monte Carlo code

Prompt gamma activation analysis (PGAA) is a nuclear analytical technique for non-destructive determination of elemental and isotopic compositions. The principle of PGAA technique is based on detection of captured gamma-ray emitted from an analytical sample while being irradiated with neutrons. Use of a cold neutron beam guide greatly reduces the gamma-ray background at the analytical sample while maintaining a neutron capture rate is comparable to that of standard thermal neutron PGAA. A new cold neutron induced prompt gamma activation analysis (CN-PGAA) system has been under construction since April of 2009 at the HANARO Cold Neutron Building (KAERI, Republic of KOREA). In this study, the Compton suppression factor of the CN-PGAA system was estimated to be 5.5 using a ⁶⁰Co radioactive source in conjunction with the MCNPX simulations. Several parameters of the CN-PGAA system were studied to estimate and optimize the performance of the system: scintillation material in the guarded detector of a Compton suppression spectrometer (CSS); the relative positions of the HPGe detector and annular detector; and the distance between the HPGe detector and back catcher BGO detectors of the CSS. In addition, the neutron ray-trace simulation package, McStas, was adopted to predict the neutron flux and wavelength distribution at the end of the cold neutron beam guide. These results served as input for the MCNPX simulation of the CN-PGAA system.     

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 multi-detector integrated automation system of routine INAA

An integrated automation system of routine instrumental neutron activation analysis (INAA) with three HPGe detectors has been built at China Institute of Atomic Energy. This system is mainly composed of sample counting system, pneumatic transfer system, software control and analysis systems, etc. The characteristics include more than 200 samples can be controlled for a batch of INAA with three detectors simultaneously, sample counting position can be optimized automatically according to the counting dead time, the real-time tracking and the high consistency between the spectrum and counting sample are possible to be realized through radio frequency identification tag.

     

Stability of metallofullerenes following neutron capture reaction on the metal ion

To achieve the highest possible sensitivity of analysis for environmental samples it is common practice to use both a high efficiency detector and a close measurement geometry with a large sample size (e.g. Marinelli beaker). Under such conditions, the typical efficiency calibration procedure results in a biased activity value for many nuclides due to the true coincidence summing effect. While there are a few methods to correct for this effect with special calibration standards, such calibrations can be both time consuming and expensive. Due to these calibration difficulties, the true coincidence summing effect is often simply ignored. Recently, it has been demonstrated that the coincidence summing correction can be performed mathematically even for voluminous sources. This new method consists of an integration of the coincidence correction factor over the sample volume while taking into account its chemical composition and the container. In this paper, we will discuss the latest approaches for establishing the peak efficiency and peak-to-total efficiency curves, which are required for this method. These approaches have been tested for HPGe detectors of two different relative efficiencies.     

Improved performance in germanium detector gamma-spectrometers based on digital signal processing

In an HPGe spectroscopy system, Digital Signal Processing (DSP) replaces the shaping amplifier, correction circuits, and ADC with a single digital system that processes the sampled waveform from the preamplifier with a variety of mathematical algorithms. DSP techniques have been used in the field of HPGe detector gamma-ray spectrometry for some time for improved stability and performance over their analog counterparts. Recent developments in HPGe detector construction and new liquid nitrogen-free cooling methods have resulted in HPGe detectors which are better adapted to the needs of the application. Some of these improvements in utility have degraded the spectroscopy performance. With DSP, it is possible to reduce the changes, in real time, in several aspects of detector performance on a pulse-by-pulse basis, which is not possible in the old analog environment. In the past, in designing for the analog regime, flexibility was limited by issues of component size, number and cost. In the digital domain, the problem translates to the need for a DSP with enough speed and an efficient algorithm to achieve the desired transformation or correction to the digitally determined pulse shape or height, event-by-event. The use of DSP allows the peak processing to be tuned to the preamplifier peak shape from the detector rather than being set to an average value determined from several detectors of the type in question. The selection of the filter can be automatic or manual. The following corrections are now possible: ballistic deficit correction, peak resolution improvement by reducing the impact of microphonic noise, increase throughput by reducing pulse processing time, and loss-free (zero dead time) counting.     

Radioxenon production through neutron irradiation of stable xenon gas

The Spectral Deconvolution Analysis Tool (SDAT) software was developed to improve counting statistics and detection limits for nuclear explosion radionuclide measurements. SDAT utilizes spectral deconvolution spectroscopy techniques and can analyze both β–γ coincidence spectra for radioxenon isotopes and high-resolution HPGe spectra from aerosol monitors. The deconvolution algorithm of the SDAT requires a library of β–γ coincidence spectra of individual radioxenon isotopes to determine isotopic ratios in a sample. In order to get experimentally produced spectra of the individual isotopes, we have irradiated enriched samples of ¹³⁰Xe, ¹³²Xe, and ¹³⁴Xe gas with a neutron beam from the TRIGA reactor at The University of Texas. The samples were counted in an Automated Radioxenon Sampler/Analyzer (ARSA) style β–γ coincidence detector. The spectra produced show that this method of radioxenon production yields samples with very high purity of the individual isotopes for ^131mXe and ¹³⁵Xe and a sample with a substantial ^133mXe to ¹³³Xe ratio.     

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.     

List-mode coincidence data analysis for highly selective and low background detection of gamma-nuclides in activated samples

Highly selective and sensitive γ-ray detection was performed by coincidence and anticoincidence event analysis after list-mode data acquisition using an HPGe spectrometer equipped with NaI(Tl) and plastic scintillation detectors. In order to obtain the most suitable detection of specific nuclides, coincidence or anticoincidence spectra could be freely constructed by extracting events with particular time and energy correlations. Although the detector arrangement of this system was the same as that of a typical Compton suppression spectrometer, background counts were drastically reduced and γ-rays of particular nuclides could be selectively detected by using γ-γ, γ-X, γ-X-X, and γ-β⁺ coincidences.     

Aktivierungsanalytische Bestimmung Extrem Niedriger Elementkonzentrationen in Reinsten Stoffen

A survey of problems connected with the activation analysis of extremely pure materials is given. The treatment of the surface of the samples influences the results. The detection limit of counting radiochemically pure nuclides are determined by efficiency, background and counting interval. The background, which usually is reduced by selected construction materials, large shields and anticoincidence techniques also may be reduced by the βγ-coincidence technique. It is possible to arrange several small β-ray detectors closely to one large γ-ray detector. Several samples are measured at the same time with a long counting interval without interferences. The method was applied to the analysis of semi-conductor silicon.     

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.     

High Sensitive Measurements of 137Cs and Other Radionuclides in Environmental Samples Using Germanium Detectors

Three types of high-purity germanium (HPGe) detector systems for low-level radioactivity measurement were constructed in the laboratory near sea level. An anti-Compton system was set up by combining a large volume HPGe (rel. eff. 115%) with a well type NaI(Tl). The detection limit (D.L.) of ¹³⁷Cs of an ashed oyster sample for the anti-Compton mode of 115% Ge was 0.023 Bq/sample for 8·10⁴ s counting, whereas 0.035 Bq/sample for the normal mode. Under similar measuring conditions, D.L. of ¹³⁷Cs for a medium volume HPGe (rel. eff. 51%) was 0.042 Bq/sample. A low-background Ge-LEPS (Low Energy Photon Spectrometer) was sufficiently sensitive for low level measurements of ²¹⁰Pb, ²³⁴Th and other low energy gamma-emitters. The detection limit for ²¹⁰Pb in the sample shape of 60 mm diameter by 2 mm thick was about 0.05 Bq/sample for 5.0·10⁵ s background counting. Using this LEPS, it was found that ²¹⁰Pb behaves similarly to ⁷Be in both air and precipitation (snowfall).