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.     

Using Monte Carlo methods to estimate efficiencies of gamma-ray emitters with complex geometries

In the event of a radioactive disaster, one of the biggest tasks is to estimate the radiation dosage received by people to determine the actions of emergency response teams. The first and the most rapid screening method of internally contaminated people in case of an emergency response is to perform in-vivo measurements for gamma-emitters. Development of virtual gamma-ray calibration techniques will be critical for emergency invivo measurements because there are inadequate numbers of phantom types to approximate all body shapes and sizes. The purpose of this project was to find a reliable way to estimate the efficiency of gamma-systems using Monte Carlo computations, and to validate that efficiency by making measurements of a standard geometry. Two geometries, a 5-ml ampoule and a Bottle Manikin Absorption (BOMAB) phantom head, spiked with ⁶⁷Ga were used as standard geometries. The radioactive objects are measured at a number of distances from a high purity germanium (HPGe) detector, and the experimental efficiency for our gamma-spectrometry system is determined. The same set of experiments was then modeled using the Monte Carlo N-Particle Transport Code (MCNP). The conclusion of this project is that computationally derived detector efficiency calibrations can be comparable to those derived experimentally from physical standards.     

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.     

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.     

Preparation and Pharmacokinetic Evaluation of Iodine-125 Labeled Alphamethyl-L-Tyrosine

A prompt gamma-ray neutron activation analysis (PGNAA) system was used to calibrate and validate a Monte Carlo model as a proof of principle for the quantification of chlorine in soil. First, the response of an n-type HPGe detector to point sources of ⁶⁰Co and ¹⁵²Eu was determined experimentally and used to calibrate an MCNP4a model of the detector. The refined MCNP4a detector model can predict the absolute peak detection efficiency within 12% in the energy range of 120–1400 keV. Second, a PGNAA system consisting of a light-water moderated ²⁵²Cf (1.06 g) neutron source, and the shielded and collimated HPGe detector was used to collect prompt gamma-ray spectra from Savannah River Site (SRS) soil spiked with chlorine. The spectra were used to calculate the minimum detectable concentration (MDC) of chlorine and the prompt gamma-ray detection probability. Using the ²⁵²Cf based PGNAA system, the MDC for Cl in the SRS soil is 4400 g/g for an 1800-second irradiation based on the analysis of the 6110 keV prompt gamma-ray. MCNP4a was used to predict the PGNAA detection probability, which was accomplished by modeling the neutron and gamma-ray transport components separately. In the energy range of 788 to 6110 keV, the MCNP4a predictions of the prompt gamma-ray detection probability were generally within 60% of the experimental value, thus validating the Monte Carlo model.     

A new highly efficient set-up for cyclic and pseudocyclic short time activation analysis with high count rates

A new counting geometry with a simple sample changer was constructed to enable cyclic and pseudocyclic short-time activation analysis. With the new system it is possible to cycle a sample, or successively an indefinite number of samples up to 20 times. The sample changer acts at the same time as sample catcher for two n-type HPGe detectors and can release the sample into a well-type HPGe detector. The new system enables the simultaneous counting of the irradiated samples by means of two endcap HPGe detectors, and subsequent counting by means of the well HPGe detector or both detector types. A well detector ensures a high counting efficiency which improves the sensitivity of a large number of short lived nuclides. Some standard reference materials (i.e., BCR-176, NIST SRM 1633b, IAEA-336, 335b, 335c) were prepared and analysed in replicates. The results indicate that up to 46 nuclides can be determined in BCR-176 if the samples are irradiated with and without the⁶LiD converter. An automatic evaluation programme was developed that determines the FWHM calibration parameters for each spectrum for accurate peak-area estimation at high count rates.     

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.     

Radioactivity levels in peloids used in main Cuban spas

In this work, an approach for determining both the outer dead layer thickness of the p-type coaxial HPGe detector and the inner dead layer thickness of the n-type coaxial HPGe detector was proposed by using two full energy peak area count ratios of a X-ray and a gamma ray emitted from the same radioisotope of ¹³⁷Cs. Monte Carlo calculations and experimental measurements were conducted to determine these dead layer thicknesses. The results showed that the outer dead layer thickness reached 0.57 ± 0.03 mm on 06 Jan 2017 after nearly 3 years of use for the p-type detector. The inner dead layer thickness reached 1.21 ± 0.24 mm on 01 Aug 2016 after more than 3 years of operation for the n-type detector. Simulation model with the modified dead layer thicknesses was used to estimate full energy peak efficiencies and gamma spectra from seven radioactive sources. The results were in good agreement with the corresponding experimental values in the gamma energy region of interest.     

K 0-prompt gamma ray activation analysis for estimation of boron and cadmium in aqueous solutions

K ₀-PGAA (prompt gamma activation analysis) has been used to estimate boron and cadmium contents in industrial and environmental materials from some different local areas as well as, samples from different locations in Burullus and Qarun Lakes. A high efficiency Compton background suppression gamma-ray spectrometry by anti-coincidence counting with a NaI(Tl) shield around a central HPGe detector for in beam PGAA using a ²⁵²Cf neutron source has been calibrated and described in this paper. The facility is principally designed for measurement of the prompt gamma-ray spectra obtained due to thermal neutron capture using 1951.14 keV gamma line of ³⁵Cl as the internal mono-standard comparator. A calibration curves were developed in which a set of boron and cadmium standards were tested and the count rate to boron and cadmium mass curves were determined. This set of boron and cadmium measurements was compared with a method for determining composition using K ₀-PGAA. Conventional prompt neutrons capture Gamma-ray results were in a good agreement with the data obtained by K ₀-PGAA method. Detection limits and self-shielding study are presented.     

A two-point in situ method for simultaneous analysis of radioactivity in seawater and sediment

A new in situ radioactivity analysis method was developed to determine the fractional contributions of gamma-ray emitters in seawater and sediment from total measured counts. A semi-empirical formula to determine the fractional count contributions was derived using the variation characteristics of the gamma-ray attenuation rate and geometrical efficiency with the measurement points. The proposed method was employed to make in situ gamma-ray measurements using a CeBr₃ detector for radioactivity analysis of seawater and sediment at a coastal area with a relatively high tidal range. The full energy peak efficiency of the detector at measurement site was obtained using the GEANT4 simulation code. The radioactivity concentration of ⁴⁰K in seawater and sediment was determined using the proposed method and laboratory analysis with sampling. The MDA of the in situ measurement for ¹³⁷Cs and ¹³¹I was also estimated assuming they were deposited on the sediment surface-layer. The validation of this method was demonstrated by comparing with the sampling analysis results.

     

Gamma-Ray Emission Probabilities in the Decay of 226Ra and Its Daughters

Relative gamma-ray emission probabilities in the decay of ²²⁶Ra and its decay products have been measured using a HPGe detector. The resulting data have been evaluated together with five previously published sets of ²²⁶Ra gamma-ray emission probabilities.     

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.     

Comparison of irradiated foil measurements with activation calculations and HPGe simulations

Theoretical activation calculations for Fe, Ni, and stainless steel foils were compared against irradiated foil measurements from a critical assembly. Calculated/experiment values spanning 0.62–1.31 showed that the restricted approach used here is insufficient for experiment planning, with the collapsed cross-section being the primary source of error. The effect of decay time on gamma-ray spectroscopy measurement reliability was investigated using a Monte Carlo HPGe detector model. Simulations showed no correlation with decay time, absent interferences. Specific interferences for Fe-59 (Ni) and Co-60 (stainless steel) activation product ratios suggested optimal measurement windows having respective decay times of 9–11 days and 4–7 days.     

A simple and economic method for accurate determination of the energy peak efficiency of 208 keV γ-ray of 237U based on 241Pu/237U secular equilibrium

A new method is developed for the determination of energy peak efficiency of 208 keV γ-ray of ²³⁷U based on ²⁴¹Pu/²³⁷U secular equilibrium. Plutonium solution was purified to remove Am with Dowex 1 × 2 anion exchange chromatography and the concentration of ²⁴¹Pu in the purified solution was determined using ²⁴²Pu isotope-dilution mass spectrometry on an inductively-coupled plasma mass spectrometry. The solution can be used as calibration source for the determination of energy peak efficiency of 208 keV γ-ray of ²³⁷U after 48 days. The method was validated for a planar HPGe detector at the 12 mm above the detector surface. The results showed that this is a simple and economic method for determining the energy peak efficiency of gamma detectors for 208 keV γ-ray of ²³⁷U.     

Full energy peak efficiency calibration of HPGe detector for point and extended sources using Monte Carlo code

Monte Carlo simulation is important to get efficiencies for cases where the experimental efficiencies are difficult to get such as for samples with nonstandard geometries and for large samples. In this paper, efficiency of the HPGe detector, routinely used in our lab for a variety of samples, has been computed for point source geometry and its parameters has been optimized to match MCNP and experimental efficiencies within 5% at different sample to detector distances. This optimized geometry was then validated by efficiency transfer to other geometries.     

The efficiency calibration of radioxenon isotopes of inhomogeneous adsorption column for HPGe γ spectrometry

In this paper, a new efficiency calibration scheme is proposed for the inhomogeneous adsorption column, in which the segment efficiencies modeled by the Monte Carlo toolkit Geant4 are weighted according to the fraction distributions of the adsorbed radioxenon based on the equilibrium adsorption theory. In order to verify the scheme, an experiment of efficiency calibration of HPGe detector by employing radon daughters was performed, and as a result the relative errors between the measured value and simulated value was less than ±?2.3%. This method developed in this paper is useful for the development of rapid test device of radioactive gas.     

Production of 152,154Eu mixed sources for calibrations of gamma-ray spectrometers

Mixed gamma-ray point sources consisting of ¹⁵²Eu and ¹⁵⁴Eu were prepared from a solution of EuCl₃ containing both isotopes. Gamma-rays emitted from these isotopes were used to establish the relative efficiency curves of HPGe detector, which were converted to absolute ones using gamma-ray sources of well-known activities. Gamma-ray attenuation correction factors were taken into account. Accuracies of activity measurements of the prepared sources were checked by measuring other sources of well-known activities and confirmed by simulating the absolute efficiency curve at distance of 15?cm from the detector window using the DETEFF software. The prepared sources were then submitted to quality control tests.     

Design of an on-line monitoring system for radioactive wastewater

An on-line monitoring system for radioactive wastewater was designed to discriminate the type and concentration of the radionuclides discharged from nuclear facilities. An HPGe semiconductor was used as the detector in the system for continuous monitoring by pumping wastewater. The minimum detectable activity for ¹³⁷Cs was 0.4 Bq L⁻¹ after 10 min of measuring wastewater with the system. The system can detect excessive radioactivity in the wastewater and quickly and effectively alert personnel. Based on the experimental measurements and the Monte Carlo simulation, the detection efficiency of the system was calibrated, and an efficiency curve was determined for the energy range from 50 to 2754 keV.

     

On the design and installation of a Compton–suppressed HPGe spectrometer at the Budapest neutron-induced prompt gamma spectroscopy (NIPS) facility

An important aspect of the ongoing upgrade at the Budapest PGAA-NIPS facility has been the design and installation of a second Compton-suppressed gamma spectrometer. The aim was to provide excellent spectroscopic conditions for future position sensitive and large sample prompt gamma activation analysis applications. The optimum geometry of the setup was determined by Monte Carlo calculations with the MCNP-CP code. The suppression factors for various layouts (co-axial, perpendicular), shapes (cylindrical, tapered), and thicknesses were compared at different gamma-ray energies. The optimum configuration, as a trade-off between performance and cost, was selected, purchased, and installed. Several characteristic features of a collimated, Compton-suppressed system could be revealed, which allowed us to achieve a better and cost-effective performance. The calculations were validated with a ¹⁴N(n,γ)¹⁵N calibration source.     

Improved radioxenon gamma-spectrometry counting system and its efficiency calibration: Monte Carlo simulation and experimental results at enriched xenon counting environment

To give satisfactory efficiency both for X- and gamma-ray photon, an improved counting system has been developed in CTBT Canadian radioxenon laboratory. The counting system consists of a BEGe detector coupled with a thin carbon fiber window counting cell, that can perform a reliable and efficient radioxenon measurement. A semi-empirical calibration procedure was adopted, which is a combination of experimental measurement and mathematical simulation. Mathematical calibration tool is Monte Carlo simulation software named VGSL. Advanced gamma-spectrum analysis software, named Aatami, was used for gamma-ray peak shape fitting and X-ray multiplets deconvolution. The calculated full energy peak efficiency curve covers from 30 to 700 keV and agrees well with experimental data points within 2%. The efficiency curve can provide radioxenon analysis both for X-rays and gamma-rays with high quality. The efficiency distortion near xenon k-absorption edge of 35 keV, which is caused by high concentrated xenon in the counting cell, is also discussed.