Evaluation of interferences on measurements of 90Sr/90Y by TDCR Cherenkov counting technique

A study to evaluate conditions affecting the determination of ⁹⁰Sr/⁹⁰Y activities in liquid samples by the triple-to-double coincidence ratio (TDCR) Cherenkov counting technique was conducted. The Cherenkov radiation produced by the ⁹⁰Y beta decay was determined using a commercially available Hidex 300 SL liquid scintillation counter. The interferences of sample geometry, including sample counting vial type and volume composition, and sample colour on the TDCR were investigated. The effects of potentially interfering beta and mixed beta–gamma emitters on the TDCR Cherenkov counting of ⁹⁰Sr/⁹⁰Y activities were also examined. The TDCR values were used to quantify counting efficiencies of ⁹⁰Y under different experimental conditions. The results demonstrated that the Cherenkov counting efficiency of ⁹⁰Y is independent of sample volume and counting vial size. The effect of colour quenching was examined using yellow and brown food-grade dyes. The TDCR correction for colour quenching was found to be effective. An evaluation of counting efficiency of different beta-emitting radionuclides demonstrated that strong gamma emissions can contribute to the Cherenkov counting efficiency. Overall, measured radioactivity values deviated from reference values by ≤7.5 %, which is acceptable for screening applications in emergency situations.     

Primary activity standardization of <Superscript>134</Superscript>Cs

Cesium-134 has been measured by means of a new coincidence counting system which is equipped with a liquid scintillation detector to count β particles and a NaI crystal to detect γ-rays which are emitted simultaneously. In order to validate this new technique, additional measurements were carried out with an established 4πβ–γ-coincidence counting system with a proportional counter in the β channel. The coincidence counting experiments were complemented with measurements in further liquid scintillation counters with two and three photomultiplier tubes. The counting efficiencies for these systems were determined using CIEMAT/NIST efficiency tracing and the triple-to-double coincidence ratio (TDCR) method, respectively.     

TDCR measurements of 3H, 63Ni and 55Fe using Hidex 300SL LSC device

The commercial Hidex LSC system has been used to measure triple to double coincidence ratio (TDCR), experimental counting efficiency (CE) and the absolute activity for radioactive standards of pure beta emitters viz. ³H, ⁶³Ni and ⁵⁵Fe, an electron capture nuclide. Colour and chemical quench measurements of ⁶³Ni and ⁵⁵Fe have been done. An excellent match between TDCR and CE has been obtained for beta emitters, while very large deviations have been observed for ⁵⁵Fe. The deviation between TDCR and experimental efficiency has been found to be nearly uniform. Based on this, an empirical correction factor for TDCR which gives the correct efficiency has been evaluated, to enable efficient application of this commercial instrument for ⁵⁵Fe estimation. These TDCR correction factors were further validated by applying for ⁵⁵Fe activity measurements in ASTM standard steel samples irradiated to a fixed neutron flux in research reactor CIRUS. Finally, ⁵⁵Fe activity in steel sample from APSARA reactor decommissioning waste was successfully estimated using this modified TDCR.     

Rapid determination of 90Sr/90Y in water samples by liquid scintillation and Cherenkov counting

Strontium-90 (⁹⁰Sr) is a ubiquitous contaminant at nuclear facilities, found at high concentrations in spent nuclear fuel and radioactive waste. Due to its long half-life and ability to be transported in groundwater, an accurate method for measuring ⁹⁰Sr in water samples is critical to the monitoring program of any nuclear facility. To address this need, a rapid procedure for sequential separation of Sr/Y was developed and tested in groundwater samples collected from an area of riverbed affected by a ⁹⁰Sr groundwater plume. Sixteen samples, plus spike and water blanks, were analyzed. Five different measurements were performed to determine the ⁹⁰Sr and yttrium-90 (⁹⁰Y) activities in the samples: direct triple-to-double-coincidence ratio (TDCR) Cherenkov counting of ⁹⁰Y, liquid scintillation (LS) counting for ⁹⁰Sr following radiochemical separation, LS counting for ⁹⁰Y following radiochemical separation, Cherenkov counting for ⁹⁰Y following radiochemical separation and LS counting of the Sr samples for ⁹⁰Y in-growth. The counting was done using a low-level Hidex 300SL TDCR counter. Each measurement method was compared for accuracy, sensitivity and efficiency. The results following Cherenkov counting and radiochemical separation were in very good agreement with one another.     

Validation of chemical separation method for the determination of 63Ni using TDCR technique in steel samples of APSARA reactor

Activity Standards of ⁶³Ni was used to benchmark our triple-to-double coincidence ratio (TDCR) primary standardization instrument Hidex 300SL TDCR device under different chemical and colour quench conditions. The results were compared with a secondary standardization instrument Tricarb 2910TR that employs transformed spectral index of external standard to assess the quench level of samples. Excellent agreement was observed (within 3 %) for a wide range of standard activity and quench conditions. The method was subsequently used for validating chemical separation procedure for estimation of ⁶³Ni in neutron activated standard nickel and steel samples. Further the method was applied for estimation of ⁶³Ni from decommissioning waste of a research reactor, APSARA.     

Activity determination of <Superscript>88</Superscript>Y by means of 4πβ(LS)-γ coincidence counting

The activity concentration of an ⁸⁸Y solution was measured by means of a new custom-built 4πβ(LS)-γ coincidence counting system. Efficiency variation was carried out using chemical quenching and neutral density filters. A relative uncertainty of 0.57% was obtained for the activity concentration. Details of the measurements and of the analysis, as well as possibilities to reduce the uncertainty are discussed. Additional validation measurements were carried out by means of the well-established coincidence counting technique using a proportional counter (PC) in the β channel. The results of both coincidence methods were found to be in excellent agreement.     

Simultaneous determination of Ir and Se in K-T boundary clays and volcanic sublimates

Our instrumental analytical method for an ultra-sensitive determination of Ir and Se in sediments and volcanic emission products is based on epithermal neutron activation analysis (ENAA) coupled with multiparameter coincidence spectrometry. An adequate setting of the energy paths and of the multiparameter coincidence spectrometry. An adequate setting of the energy paths and of the multiparameter analyzer allows a simultaneous counting of⁷⁵Se and¹⁹²Ir coincidences. This tool has been used to analyse different sediments sampled at the Cretaceous-Tertiary boundary (KTB) and volcanic samples in order to discuss the extra-terrestrial or volcanic origin of the Ir anomaly.     

Geant4 Monte Carlo radioxenon beta-gamma coincidence efficiency simulation for a phoswich detector

In this work, a Monte Carlo (MC) simulation model is established to accurately characterize a phoswich beta-gamma coincidence detector system. This model can be easily used to predict the beta-gamma coincidence efficiencies of xenon radioisotopes at various stable xenon concentrations in the counting cell. The results demonstrate that there is a significant inverse correlation between beta-gamma coincidence efficiency and stable xenon concentration. The influence of stable xenon concentration on beta-gamma coincidence counting efficiency has been investigated for each individual xenon radioisotope. The results indicate that the effect of stable xenon concentration on beta-gamma coincidence efficiency depends on the xenon radioisotope and its decay modes. The coincidence efficiency of ¹³³Xe with 31.0-keV X-ray decay mode is the most affected one; and then followed by ^131mXe, ¹³³Xe with 81.0-keV gamma-ray decay mode, ^133mXe and finally ¹³⁵Xe. The study also indicates that the gamma absorption by xenon gas plays more of a role in the decrease of beta-gamma coincidence efficiency for ¹³³Xe and ¹³⁵Xe, and that the conversion electron spectrum shifting and broadening plays more of a role in the reduction of beta-gamma coincidence efficiency for the metastable radioxenon of ^131mXe and ^133mXe.     

Activity standardization of <Superscript>99m</Superscript>Tc using liquid scintillation counting method

The Korea Research Institute of Standards and Science (KRISS) participated in the BIPM.RI(II)-K4.Tc-99 m comparison of activity measurements of ^99mTc. We develop the national primary standard for ^99mTc solution used during the comparison. We use two primary liquid scintillation counting techniques for the standardization: digital coincidence counting with the 4πβ(LS)-γ(NaI(T1))system and triple-to-double coincidence ratio counting. Both methods give consistent results for the specific activity of a ^99mTc solution. Adopting the result from the DCC method as the reference value of the ^99mTc measurement, we evaluate the standard uncertainty of 0.856% for the KRISS primary standard of the ^99mTc activity. The K4 comparison result shows that the newly-established KRISS primary standard lies within the standard uncertainty with the key comparison reference value defined from other ^99mTc measurements.     

Degradation of 81 keV <Superscript>133</Superscript>Xe gamma-rays into the 31 keV X-ray peak in CsI scintillators

Pacific Northwest National Laboratory uses beta-gamma coincidence detectors in a number of xenon sampling and measurement systems to enable simultaneous, sensitive measurements of ¹³¹Xe, ¹³³Xe, ^133mXe, and ¹³⁵Xe for treaty monitoring applications. In recent years, a new style of beta–gamma detector was developed to improve upon the detector module used in the Automated Radioxenon Sampler/Analyzer. The results of an MCNP5 Monte Carlo simulation of the new detector cell are presented, with particular emphasis on the identification of an energy deposition sequence with the potential to introduce significant error into the detector efficiency calibration. This sequence occurs when an 81 keV gamma from ¹³³Xe is absorbed in an inactive region of the CsI(Na) scintillator, followed by emission of a 31 keV X-ray from cesium (or possibly a 28.5 keV X-ray from iodine). These X-rays add excess counts into the 31 keV peak observed in the decay of ¹³³Xe. The impact of this effect on different efficiency calibration techniques is discussed.     

Automated production of 64Cu prepared by 18?MeV cyclotron

⁶⁴Cu (T_1/2?=?12,7?h, ??^? 37,1?%, ??⁺ 17,9?%, EC 41?%) is a useful radioisotopes for positron emission tomography radiopharmaceutical. We used the reaction route ⁶⁴Ni(p,n)⁶⁴Cu for the ⁶⁴Cu preparation. A basic disadvantage of this route, a high price of the enriched target material, was eliminated by using very simple recycling procedure. Compact solid target irradiation system was installed at the end of the external beam line of the IBA Cyclone 18/9 cyclotron. In this paper, the irradiation of ⁶⁴Ni target and separation of ⁶⁴Cu from a target material is described. The separation was achieved by anion exchange chromatography with HCl as a elution solution. The distribution ratio for different HCl concentrations on Bio-Rad AG1-X8 and elution profile of ⁶⁴Cu were investigated. ⁶⁴Cu production rate for 100?mg ⁶⁴Ni of 99.09?% purity (ISOFLEX) on gold target was 104?MBq/??Ah. The activity of the product was checked by ionisation chamber (Curiementor), gamma spectrometry using a HPGe detector and liquid scintillation counting using the triple-to-double coincidence ratio method. The separation process of ⁶⁴Cu was made in a home-made separation module.     

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.     

Adaptation of PTB’s analytical modelling for TDCR–Cherenkov activity measurements at LNHB

Designed for triple to double coincidence ratio measurements based on liquid scintillation, the three-photomultipliers detection system can also be applied for Cherenkov counting using aqueous solutions. For activity determination, a specific modelling of Cherenkov light emission has to be constructed. For that purpose, the analytical modelling first developed at PTB was adapted to account for the physical features of the detection system used at LNHB. The first results are presented in the case of activity measurements of two high-energy β^?-emitters (⁹⁰Y and ⁸⁹Sr). The analytical modelling was also tested for the standardization of ⁶⁸Ge in a solution of ⁶⁸Ge/⁶⁸Ga in equilibrium in the framework of a BIPM international comparison in 2014.     

New technique to trace [<Superscript>15</Superscript>O]water uptake in a living plant with an imaging plate and a BGO detector system

Summary We present a new trial to measure real time water movement in a living plant using the positron emitting radionuclide, ¹⁵O. ¹⁵O was prepared by ¹⁴N(d,n)¹⁵O reaction and 10 ml of ¹⁵O labeled water (2 GBq) was supplied from the root of a soybean plant. To detect activity, an imaging plate (IP) as well as a BGO detector system were used. Since the half-life of ¹⁵O is extremely short, (T_1/2= 122 s), water uptake measurement was performed only for 20 minutes. In order to get [¹⁵O]waterimage, an IP was exposed to the plant for 1 minute for two times. Since the exposure to an IP requires dark condition, a BGO detector system was developed to measure [¹⁵O]waterunder light condition. A couple of BGO probes was set at the lowest stem and the gamma-rays (0.511 MeV) emitted from the radionuclide were measured through coincidence counting and compared with the radioactivity measured from an IP image. Using this system, we have found that the water uptake activity of the plant was drastically reduced under high humidity (99%) and dark condition.     

Determination of 131mXe and 133mXe in the presence of 133gXe via combined beta-spectroscopy and delayed coincidence

The International Monitoring System for the Comprehensive Nuclear-Test-Ban Treaty will include measurements of Xe fission products. Pacific Northwest National Laboratory has developed an automated system for separating Xe from air which detects Xe fission products using a beta-gamma counting system for ^131mXe, ^133mXe, ^133gXe, and ^135gXe. Betas and conversion electrons are detected in a plastic scintillation cell containing the Xe sample. Gamma and X-rays are detected in a NaI(Tl) scintillation detector which surrounds the plastic scintillator sample cell. Two-dimensional pulse-height spectra of gamma-energy versus beta-energy are obtained. The plastic scintillator spectrum in coincidence with the 31-keV X-rays from ^131mXe. ^133mXe, and ^133gXe is a complex mixture of conversion electrons and betas. A new technique to simultaneously measure the delayed coincidence (T _1/2 = 6.27 ns) between beta-particles from ^133gXe and conversion electrons depopulating the 81-keV state in 133 Cs is being developed. This technique allows separation of the ^133gXe beta spectrum from the conversion electrons due to ^131mXe and ^133mXe and uniquely quantifies all three nuclides.     

New concepts for radiometric measurements of environmental samples

The Radiation Detection and Nuclear Sciences Group at Pacific Northwest National Laboratory has a long history in conducting measurements of radioisotopes for various applications. This experience includes ultra-low background measurements, arrays of germanium detectors, automated sampling and measurement systems and coincidence measurement systems. A recent lab-supported effort has been studying how these capabilities, both in terms of hardware and experience, can be leveraged to enable environmental sampling measurements. One area of interest is the release of fission products and actinides into the environment from a reactor incident. While the initial survey of this area is still under way, one isotope of interest that surfaced early in the study is ²³⁸Pu. Existing techniques to assay this isotope suffer from measurement challenges. In alpha counting, there can be significant interference with ²⁴¹Am, while in mass spectrometry, there can be interference with ²³⁸U. The authors are developing the concept for a detector that through coincidence counting techniques can distinguish ²³⁸Pu and ²⁴¹Am. In addition, we will design the system to conduct radiometric measurements of other plutonium isotopes to enable a direct comparison of those isotopes. We will present our concept of the detector system for ²³⁸Pu, as well as discuss other radiometric measurements of fission products and actinides with which we intend to advance the state of the art for environmental measurements.     

Simple and rapid methods for on-site determination of radon and thoron in soil-gases for seismic studies

The determination of soil-gas anomalies especially ²²²Rn anomalies, are important to precisely locate fault traces, as well as to investigate earthquake precursors. In this paper, we have studied and compared new rapid methods for on site determinations of radon (²²²Rn), thoron (²²⁰Rn) and total radon (²²²Rn+²²⁰Rn) in soil-gas. These new techniques pump the soil-gas continuously from the soil through a simple sampling tube to the counting cell for one-minute with discarding the excess. Then, either four one-minute counting periods (5-minute technique) or nine one-minute counting intervals (10-minute technique) are followed immediately. In all the methods, conversely to Morse"s method, the first counting period (C1) was not employed for calculations. Three calculation methods for the five-minute technique, two for the ten-minute technique and a modified Morse"s method are compared with theoretical values and different real soil-gases with different radon/thoron ratios. The affect of different flow rates of soil-gases into the counting cell was also investigated. Finally, the ten-minute technique seems to be a little more accurate, but the 5-minute technique is much more suitable for seismic field studies when a much larger number of determinations are required in a short time.     

Simultaneous determination method of radon-222 and radon-220 by a toluene extraction-liquid scintillation counter

A new determination method for²²²Rn and²²⁰Rn in water sample was developed by extracting radon with toluene and applying the integral counting method with a liquid scintillation counter. The essential characteristics of the methods are, (1) extraction of radon with toluene from water, (2) finding absolute counts and making corrections for the quenching effect by the adoption of the integral counting method, (3) the determination of²²²Rn and²²⁰Rn was performed by counting the activity of²²⁰Rn with its descendants and of ThB (²¹²Pb) with its descendants in a radioactive equilibrium, respectively, (4) realizing high sensitivity by simultaneous counting of α, β⁻ particles emitted from the decay products formed in toluene. The lowest detection limit obtained by the present method was 5.0·10⁻¹³ Ci/l for²²²Rn and 6.8·10⁻⁸ Ci/l for²²⁰Rn in water.     

Comparison of the Precision and Accuracy of Digital Versus Analogue Gamma-Ray Spectrometric Systems Used in INAA for Evaluation of Homogeneity and Certification of Reference Materials of the IAEA

Performance of three commercial gamma-ray spectrometric systems was evaluated for precision and accuracy prior to use in characterization of reference materials. Two of the systems were based on fast processing of the analogue signal from the amplifier (EGG Ortec model 672) using a loss free counting module (Canberra model LFC 599) interfaced to one of two analog-to-digital converters (Canberra models 8713 or 8715). The third system was based on a digital signal processor (Canberra model DSP 9660). Performance of the systems was tested over a range of count rates up to a maximum of 70,000 counts per second (dead time up to 90%) using ⁶⁰Co and ¹³⁷Cs sources. Best resolution was achieved with an analogue system with ADC 8713. The analytical results obtained with the digital system show the lowest and well-quantified uncertainty.     

Radioactivity measurement and standardization in Thailand

An absolute measurement method for disintegration rates of radioisotopes by 4p beta-gamma coincidence counting systems is described. Absolute activity of ⁶⁰Co and ⁹⁹Mo was determined by the counting systems of Japan and Thailand. Radon gas measurement and standardization were also performed. A radon chamber was constructed and employed for the comparative measurements by a pulse-counting ionization chamber and an environmental-level scintillation chamber. The background radon concentration of the radon chamber was also determined.