Monte Carlo characterisation of a Compton suppressed broad-energy HPGe detector

GEANT4 Monte Carlo simulations have been successfully utilised to characterise a Compton suppressed broad-energy HPGe detector. The detector setup has been fully recreated in the simulation, which has been optimised to consistently reproduce the detector response. The peak efficiencies for both the primary BEGe detector and NaI(Tl) guard detectors agree with the simulated values for multiple test sources within 3 %. Compton suppression has also been simulated, with good agreement seen between the simulated and actual CSF values (<10 %) for multiple radionuclides. A secondary reference source was also simulated, which contained up to 30 radionuclides in a different geometry to that of the previous source. This showed excellent agreement with experimental data in both unsuppressed and suppressed modes of operation.     

Thin layer spectroelectrochemical (RVC-OTTLE) studies of pertechnetate reduction in acidic media

A Peltier-cooled silicon drift detector was successfully applied for conversion electron spectrometry. The energy resolution of the detector for 45 keV electrons was 0.50 keV (FWHM). The approximate thickness of the dead layer was determined to be 140 ± 20 nm Si equivalent. The relative efficiency of the detector was verified to be approximately constant in the energy range of 17–75 keV. This is concordant with the high transparency of the thin dead layer and the sufficient thickness of the detector (450 μm) to stop the electrons. The detector is suitable for use in plutonium analysis of chemically prepared samples. Moreover, it was demonstrated that conversion electron spectrometry is better than alpha spectrometry in preserving its capability to determine the ²⁴⁰Pu/²³⁹Pu isotopic ratio as a function of sample thickness. The investigated measurement technique can be considered a promising new tool in safeguards, complementary to existing methods.     

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.     

AutoCal: a method for automatic energy calibration of β–γ systems based on a 137Cs spectrum

A method was developed and implemented that calculates energy versus channel calibrations. This method utilizes a ¹³⁷Cs spectrum acquired in β–γ coincidence. Both the γ singles and the β–γ coincident spectrum are utilized. The γ singles spectrum is utilized to calculate the γ detector energy versus resolution function. The Compton line in the β–γ coincidence is then used to calculate the β detector energy versus resolution function. Currently a linear regression (y = mx + b) is utilized to fit the data. However, higher order polynomials may easily be implemented if desired.     

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.     

A well-type phoswich detector for nuclear explosion monitoring

In this work, a well-type phoswich detector with three scintillation layers has been designed and tested for measuring atmospheric xenon radioisotopes in order to monitor nuclear explosions. The detector was made by optically coupling three concentric cylindrical scintillation layers (BC-400, CsI(Tl) and BGO) to a single photomultiplier tube. Beta-gamma coincidence technique was used to detect beta particles and gamma rays. Other important features of this detector are its Compton suppression capability and simple, compact and cost effective design. Our calculations and measurements with the well-type phoswich detector show that the minimum detectable concentrations are close to or below 1 mBq/m³ for the four xenon radioisotopes.     

Determination of isotopic ratios of uranium samples using passive gamma spectroscopy with multiple detectors

Uranium samples of various enrichments have been passively counted on the University of Texas detector gamma–gamma coincidence system. By observing gamma rays emitted from ²³⁵U and its daughters compared to gamma rays emitted by ²³⁸U daughters and comparing the data to standards of known enrichments, a technique has been developed to take a uranium sample of unknown enrichment and passively count it to determine its uranium isotopic concentration. Because the gamma rays from ²³⁵U are generally in the low-energy regime, there is a strong susceptibility to background interferences, especially from the Compton background produced from higher energy gamma rays. Other interferences, such as those from the decay series of uranium also exist for ²³⁵U gamma rays. In this light, we have collected data using list-mode to produce two-dimensional gamma–gamma coincidence spectra, which allows us to gate the low-energy gamma rays from ²³⁵U with gamma rays that are in coincidence. In doing this, much of the low energy interferences are reduced, and one can analyze the ²³⁵U gamma rays with high precision. Because of the high density of uranium, self-shielding has significant effects especially in the low-energy regime. To correct for this attenuation the detector system has been modeled by MCNP and self-shielding factors have been calculated across the energy spectrum. A big advantage to this method is the capability of performing this analysis with small (<1 g) samples in a non-destructive and relatively inexpensive manner. If necessary, this analysis can be performed within 24 h if an urgent nuclear forensics scenario arises.     

Determination of zinc in geological samples using Compton suppression with thermal and epithermal instrumental neutron activation analysis

The determination of Zn in geological samples using instrumental neutron activation analysis is usually done using the ⁶⁴Zn(n,γ)⁶⁵Zn reaction and its 244 day half-life. However this analysis has proven to be potentially difficult. This is due to its relatively low neutron absorption cross section and gamma ray intensity, and the relatively high neutron absorption cross section and gamma intensity of ⁴⁶Sc, which has an energy peak that is only 5 keV greater than ⁶⁵Zn. The use of a high resolution detector makes it possible to differentiate between the ⁶⁵Zn and ⁴⁶Sc photopeaks peaks. However, the dominating ⁴⁶Sc gamma ray can even make peak fitting routines unsuccessful in the proper determination of ⁶⁵Zn. The use of a Compton suppression system suppresses the ⁴⁶Sc peak, which has two coincident gamma-rays, and this greatly improves the ratio of the height of the ⁴⁶Sc 1120.5 keV photopeak to the ⁶⁵Zn 1115.4 keV photopeak. Irradiating the sample with epithermal neutrons also improves the measurement since ⁶⁵Zn has a higher cross section for epithermal neutrons rather than thermal neutrons, whereas ⁴⁶Sc has a higher thermal cross section. Another technique to determine zinc is the use of ⁶⁸Zn(n,γ)^69mZn reaction with its 13 h half-life using epithermal neutrons and Compton suppression INAA. However, the 438 keV gamma ray of ^69mZn has no interference with any adjoining photopeak. A critical comparison of these two methods is given.     

Determination of the calibration factor for CR-39 based indoor radon detector

CR-39 based radon detectors are widely used in measuring indoor radon. In this regard, different groups have developed their own systems. However, before using any system for indoor radon measurements, it has, first, to be calibrated with a known source of radon. In the current study, CR-39 based NRPB type radon detector has been calibrated and presented. In this regard, about 200 holders for CR-39 were obtained from the Radiation Protection Division of the Health Protection Agency (former NRPB), UK and several thousand more similar detector holders, hereafter called NRPB type holders, were fabricated locally in Pakistan. Uranium ore samples of known grade were placed into the plastic containers of volume 5.4 × 10³ cm³ and CR-39 detectors were placed in the NRPB type holders and were then installed into the containers at a distance of 25 cm from the surface of the known grade ore samples. The containers were hermetically sealed and the detectors were allowed to expose to radon for 3 weeks. After 16 h etching in 25 % NaOH at 80 °C, the measured track densities were related to the radon concentration. The calibration factor of 2.563 tracks cm^?2 h^?1/kBq m^?3 was obtained.     

Improved detector response characterization method in ISOCS and LabSOCS

The In-Situ Object Calibration Software (ISOCS) and the Laboratory Sourceless Calibration Software (LabSOCS) developed and patented by Canberra Industries have found widespread use in the gamma-spectrometry community. Using the ISOCS methodology, one can determine the full energy peak efficiencies of a germanium detector in the 45 keV-7 MeV energy range, for practically any source matrix and geometry. The underlying mathematical techniques used in ISOCS (and LabSOCS) have undergone significant improvements and enhancements since their first release in 1996. One of these improvements is  a spatial response characterization technique that is capable of handling the large variations in efficiency that occurs within a small region. The technique has been in use in ISOCS and LabSOCS releases since 1999, and has significantly improved the overall quality of the close-in and off-axis response characterization for HPGe detectors, especially for Canberra’s Broad Energy Germanium (BEGe) detectors. In this method, the detector response is characterized by creating a set of fine spatial efficiency grids at 15 energies in the 45 keV-7 MeV range. The spatial grids are created in (r,&odash;) space about the detector, with the radius r varying from 0 to 500 meters, and the angle &odash; varying from 0 to π. The reference efficiencies for creating the spatial grids are determined from MCNP calculations using a validated detector model. Once the efficiency grids are created, the detector response can be determined at any arbitrary point within a sphere of 500-meter radius, and at any arbitrary energy within the specified range. Results are presented highlighting the improved performance achieved using the gridding methodology.     

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.     

EDXRF imaging of Pb in glazed ceramics using a micropattern gas detector

A new system for energy-resolved X-ray fluorescence imaging using a microhole and strip plate (MHSP), a new type of micropattern gas detector (MPGD), is proposed. It works as a single photon counting detector with position and energy detection capability. The interaction of X-rays with the gas medium produces electrons via the photoelectric effect, and the number of electrons is proportional to the absorbed X-ray energy. These electrons are further multiplied in the MHSP. Position detection is achieved using the charge division method. The detector has an active area of 28?×?28 mm² and shows good position resolution, about σ?=?125 μm, an intrinsic energy resolution of about 14% FWHM for 5.9 keV X-rays, and a counting rate capability of up to 0.5 MHz. The system has shown good properties for energy-dispersive X-ray fluorescence (EDXRF) applications, since it allows efficient energy and position detection of fluorescence X-rays from multielemental samples. In this work, the system was used to study lead depth distributions in eighteenth-century Portuguese faiences from the Santa Clara-a-Velha monastery. The fluorescence images were obtained by irradiating the samples, with a pinhole placed between the sample and the detector to focus the radiation into the detector. The results are presented here, including the elemental map distributions for different samples.     

Self-calibration method for cerium-doped lanthanum bromide scintillator detector in the 0.1–2.0 MeV energy range

In recent years, the cerium-doped lanthanum bromide, LaBr₃ (Ce = 5 %) detector is increasingly playing an important role in radiation measurements because of its higher energy resolution (~3 % at 662 keV), faster luminescence decay time (~35 ns) and higher detection efficiency compared to 7.65 cm × 7.65 cm NaI(Tl) detector. Intrinsic spectra between 1,800 and 3,000 keV derived from internal radioactivity within LaBr₃(Ce) scintillators have been investigated in some literatures, and these results are confirmed by the experiments in this work. In this paper, a new method for LaBr₃(Ce) detector energy calibration from 100 to 2,000 keV is proposed using the intrinsic spectra (self-calibration) instead of the standard gamma sources. Proof-of-concept experiment results show that self-calibration can guarantee energy accuracy of better than 0.815 % and can be applied outside the laboratory. The stability and applicability of this method are also investigated systematically.     

Single crystal HPGe (80%) versus BGO shielded CLOVER detector for high precision decay rate measurements: a comparative study

In this study, various detector configurations have been investigated in order to explore the optimal condition for decay rate measurements of radioactive samples using gamma spectroscopy technique. A limitation of detecting low energy gamma rays from decaying radioactive nuclei, is the Compton background which can be significantly reduced by rejecting Compton scattered events through active Bismuth germanate (BGO) shielding. On the other hand, for a CLOVER detector without BGO shielding, one can place the radioactive samples very close to the detector for enhancing geometrical efficiency. A single crystal High Purity Germanium (HPGe) detector can also be used for decay rate measurements. In order to measure the decay rate of nuclei decaying via gamma emission with reasonable intensity, optimal close geometry options have been investigated for various HPGe detector configurations.

     

A simple method for self-attenuation correction in <Superscript>210</Superscript>Pb activity measurement in a well-type HPGe detector

A simple method for ²¹⁰Pb determination in a well-type detector for matrix with apparent densities ranging from ρ = 0.430 g cm^?3 to ρ = 2.037 g cm^?3 is presented. Ten spiked samples of ²¹⁰Pb were prepared to obtain the detector efficiency as a quadratic function of the matrix density. Then this equation was validated and successfully used to measure ²¹⁰Pb concentration activity in other samples. The equation proposed in this work is specific for each germanium detector; however it is proposed an extrapolation of the method to other well-type germanium detector by preparing a spiked sample and determining the efficiency for ²¹⁰Pb.     

Simultaneous measurement of flight time and energy of large matrix-assisted laser desorption ionization ions with a superconducting tunnel junction detector

We evaluated a cryogenically cooled superconducting Nb-Al₂O₃-Nb tunnel junction (STJ) for use as a molecular ion detector in a matrix-assisted laser desorption ionization time-of-flight (MALDI-TOF) mass spectrometer. The STJ responds to ion energy and theoretically should detect large molecular ions with a velocity-independent efficiency approaching 100%. The STJ detector produces pulses whose heights are approximately proportional to ion energy, thus the height of a pulse generated by the impact of a doubly charged ion is about twice the height of a singly charged ion pulse. Measurements were performed by bombarding the STJ with human serum albumin (HSA) (66,000 Da) and immunoglobulin (150,000 Da) ions. We demonstrate that pulse height analysis of STJ signals provides a way to distinguish with good discrimination HSA⁺ from 2HSA²⁺, whose flight times are coincident. The rise time of STJ detector pulses allows ion flight times to be determined with a precision better than 200 ns, which is a value smaller than the flight time variation typically observed for large isobaric MALDI ions detected with conventional microchannel plate (MCP) detectors. Deflection plates in the flight tube of the mass spectrometer provided a way to aim ions alternatively at a MCP ion detector.     

Simultaneous Removal of H<Subscript>2</Subscript>S and Dust in the Tail Gas by DC Corona Plasma

The removal of hydrogen sulfide and dust simultaneously by the DC corona discharge plasma with a wire-cylinder reactor was studied at atmospheric pressure and room temperature. The outlet gases were analyzed by Fourier Transform Infrared. Chemical compositions of the dust collected from ground electrode were analyzed by X-ray fluorescence. The results showed that the DC corona discharge is effective in removing H₂S and dust simultaneously. The best H₂S conversion was gained with the 2 cm discharge gap. The lower inlet H₂S concentration, the higher conversion efficiency was gained at any specific input energy (SIE), while the energy yield was on the contrary. The removal efficiency of H₂S decreased gradually as oxygen concentration increased, which means that the H₂S decomposition mainly depends on direct electron collisions or short-living species, such as^·O, ^·OH radicals in the non-thermal plasma. At the initial stage, the conversion efficiency of H₂S increased with the increasing of relative humidity, but later decreased while the relative humidity keep increasing with the same SIE. Existing of dust can not only reduce the energy consumption of H₂S conversion and improve the removal efficiency, but also inhibit the yield of SO₂ for it can further react with some compounds in the dust. With the discharge gap of 2 cm, inlet H₂S concentration of 2400 ppm, O₂ Of 0.5 %, relative humidity of 41 %, dust content of 4000 ± 5 % mg/m³ and SIE of 600 J/L, the H₂S conversion reached 98.8 %, and the dust removal efficiency was close to 100 %.     

Comparison of transfer factors of <Superscript>137</Superscript>Cs from soil to leafy vegetables in pot experiment and ambient environment

The paper deals with the transfer factors (TF) generated for a few varieties of leafy vegetables (spinach, fenugreek, and amaranths) consumed by the locals around Tarapur atomic power station environment in India. The soil and leafy vegetable samples collected from the ambient environment of nuclear site were used for the determination of the TFs and they were compared with TFs generated from pot experiments under controlled conditions for ¹³⁷Cs. The activity of ¹³⁷Cs in soil and each vegetable was determined by gamma spectrometry using HPGe detector (35 and 160% relative efficiency) and was reported on dry weight basis for both ambient environment and pot samples. The radioactive effluent containing ¹³⁷Cs (pH ~7) from nuclear power station was used to spike the soil for pot (size 90 cm × 45 cm × 42 cm) experiment. The TFs obtained for ambient environment and pot experiment were found to be in the range of 0.035–0.592 and 0.0054–0.29, respectively. It is observed that TFs of ambient environment are in good agreement with those obtained in the pot experiment conducted under controlled conditions. Further, the observed TF values at Tarapur nuclear site are comparable with the range of typical IAEA transfer factor values for general leafy vegetation (0.11–2.9) for tropical environment.     

Performance of HPGe gamma spectrometry system for the measurement of low level radioactivity

Comprehensive quality assurance/quality control procedure is very much necessary to obtain accurate and precise analytical measurement result. This paper discusses the quality control aspects of the High-Purity Germanium (HPGe) based gamma spectrometry system, which has been used for the measurement of low-level radioactivity in environmental samples. The gamma spectrometry system consisting of coaxial n-type HPGe detector having 50% relative efficiency with respect to 7.62 cm x 7.62 cm NaI (Tl), Nuclear Instrumentation Module (NIM) based pulse processing electronic accessories and 8 k MCA. To reduce the background contribution, 7.5 cm thick lead has been placed surrounding the detector. The minimum detectable activities (MDA) with 95% confidence level (for 300 g soil sample and 100,000 s counting time) for important radionuclides such as ²³⁸U, ²²⁶Ra, ²³²Th, ⁴⁰K, and ¹³⁷Cs are 10.4, 4.3, 4.1, 16.9 and 0.1 Bq kg^?1, respectively. The Quality control (X bar R) charts were plotted using ¹³⁷Cs and ⁴⁰K background counts observed periodically, which showed that the fluctuation is well within the confidence limit and confirms the stability of the system. The laboratory has been participating in the proficiency tests (PTs) of the International Atomic Energy Agency (IAEA). In recently concluded PTs, the samples include soil, spiked standard solution, spinach, phosphogypsum and spiked air filter were analysed for the natural, fission and activation products radionuclides. The performance evaluation of the IAEA PTs showed that the laboratory results were in good agreement with the target value, which confirms the reliability and traceability of the gamma spectrometric measurement result of the laboratory.     

Development of chromatographic methods by using direct-sampling procedure for the quantification of cyclic and linear volatile methylsiloxanes in biogas as perspective for application in online systems.

By empirically examining the persistent theme, we hope to produce a more complete understanding of methods for determination of volatile methylsiloxanes in biogas stream. Therefore, we made an attempt to investigate a rapid and sensitive method for simultaneous analysis of linear and cyclic volatile methylsiloxanes in sewage biogas in the context of the perspective for application in online systems. The gas chromatographic (GC) parameters were optimised, and sampling of volatile methylsiloxanes from biogas was performed using novel direct sampling procedure with applying of three kinds of liquid-media. Through application of well-established gas chromatography technique coupled with two types of detector – flamed ionisation detector and mass spectrometer detector – we developed the characterisation of the presented methods. Moreover, during the samples preparation the extraction procedure was consistently excluded, as well as the time of analysis was significantly reduced. The analyses were carried out by applying special constructed sampling train where the absorbed VMSs were trapped and analysed directly by GC technique, afterwards. The instrumental analytical protocol was found to yield a linear calibration in the range 0.1–55.13 (µg g^?1) with R² values 0.996 and in the range from 0.1 to 65.17 µg g^?1) with R² values > 0.99 for GC-FID and GC-MS method respectively. In all analysed samples linear and cyclic VMSs were found in sewage gas with quantities exceeding 4.6 mg Nm^?3 and 19.9 mg Nm^?3, respectively Furthermore, estimation of VMSs solvent absorption efficiency was tested and the highest absorption efficiency was obtained when acetone was used as a primary solvent. High range of linearity (0.1–65.17 µg/g), and low values of limit of detection (0.01 µg/g), limit of quantification (0.04 µg/g) clearly indicate that the analysis can be successfully repeated in other independent laboratory. The proposed method creates the real perspective for analyis of VMSs in on-line system.