Effect of reagent concentration on Cerenkov counting efficiency

Cerenkov counting is often regarded as a modified version of liquid scintillation counting in which chemical quenching is not manifested. However, the mechanism of Cerenkov counting is such that changes in the concentration of reagents in the counting medium results in changes in Cerenkov counting efficiency. Large changes in counting efficiency occur for nuclides with low average beta energy values (Ē_β). The percent increase in Cerenkov counting efficiency in 4M HCl (relative to water) for various nuclides was found to be a smooth function of Ē_β. The relative change in counting efficiency for²⁴Na,³²P,⁴²K and²⁰⁴Tl in HCl, NH₄Cl and/or NaCl media are presented. The data emphasizes the need to keep the concentration of various chemicals in Cerenkov counting media constant, especially for nuclides with low Ē_β, values, in order to reproduce counting efficiency.     

Distribution of137Cs in soil in Central Slovakia and fast prediction of contamination

This paper describes the measurement of²¹⁰Bi by Cerenkov counting in a commercial liquid scintillation counter. The counting efficiency in water is 0.17 counts per second per Becquerel (17%). When the enhancers Triton X-100 (15% v/v) and sodium salicylate (1% m/v) are added to the solution the counting efficiency for²¹⁰Bi increases from 17% to 75%. The²¹⁰Po daughter of²¹⁰Bi causes interference of 0.85 counts per second per Becquerel in the presence of the enhancers but not in water. When²¹⁰Bi and²¹⁰Po are present in secular equilibrium the total counting efficiency is 160%. When²¹⁰Bi and²¹⁰Po are not in secular equilibrium the²¹⁰Po can be removed immediately before counting by plating onto silver foil. The use of the enhancers gives a substantial increase in counting efficiency compared to counting in water. Compared with solutions used in liquid scintillation counting the enhancer solution is inexpensive and can be disposed of without environmental hazard.     

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.     

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.     

Design and performance of a miniature TDCR counting system

A portable liquid scintillation counting system based on the triple-to-double coincidence ratio (TDCR) method was developed at Sofia University “St. Kliment Ohridski”. The system consists of a miniature TDCR counter with cylindrical optical chamber and a specialized TDCR counting module named nanoTDCR. The nanoTDCR module is produced by the labZY company and provides several important new TDCR counting functionalities like: individual extending-type dead-time in each channel; simultaneous counting with two different extendable dead-times and two different coincidence windows and simultaneous TDCR counting and spectrum acquisition. The performance of the new system was tested in benchmark comparisons with the LNHB’s primary TDCR counting system of activity measurements of ²⁴¹Am, ³H, ¹⁴C and ⁶³Ni. Good agreement between the two systems was observed.     

Wavelet based spectrum processing for reduction of counting duration for quantitative estimation of ultra-trace activity in environmental matrices

A simple wavelet transformation based pre-processing method is employed to minimize the duration of counting for gamma spectrometric measurements of samples from environmental matrices. Among the various forms of analyzing wavelets, a suitable one is chosen for this purpose. Measurements with 55 different counting durations were subjected to the wavelet based processing and results were compared with long duration counting time measurements of ⁴⁰K, ¹³⁷Cs, radionuclide from ²³⁸U series (²¹⁴Bi, ²¹⁴Pb) and ²³²Th series (²²⁸Ac, ²¹²Bi, ²¹²Pb, ²⁰⁸Tl). It is observed that with a proper choice of the wavelet function a tenfold reduction in counting duration can be achieved with errors <5 %.     

Determination of neodymium isotopes as burnup indicator of highly irradiated (U,Pu)O2 lmfbr fuel

A new counting method was developed to determine²²⁶Ra in environmental samples by separating the equilibrated²²²Rn into a liquid scintillator. The integral counting method, which was originally developed for isolated individual radionuclides, was extended to the mixture of²²²Rn and its daughters in equilibrium. The optimum measurement conditions were established by examining the energy spectrum, counting time and quenching effect. An absolute counting was practiced by extrapolating the integral counting rate-bias voltage curve with the highest gain to zero bias. The detection limit thus obtained was 3 to 4·10⁻¹³ Ci.     

Development of a sequential method for the determination of238U,234U,232Th,230Th,228Th,228Ra,226Ra,and210Pb. in environmental samples

A sequential analytical method for the determination of²³⁸U,²³⁴U,²³²Th,²³⁰Th,²²⁸Th,²²⁸Ra,²²⁶Ra and²¹⁰Pb in environmental samples was developed. Uranium and thorium isotopes are first chromatographically sepaaated using tri-n-octyl phosphine oxide (TOPO) supported on silica gel. The uranium isotopes are determined by alpha-spectrometry following extraction with TOPO onto a polymeric membrane. Thorium isotopes are co-precipitated with lanthanum fluoride before counting in an alpha spectrometer. Radium isotopes and²¹⁰Pb are separated by co-precipitation/precipitation with mixed barium/lead sulphate. Radium-226 is determined by gross alpha counting of the final BaSO₄ precipitate and²²⁸Ra by gross beta counting of the same source. Lead-210 is determined through beta counting of its daughter product²¹⁰Bi.     

Quantification of99Tc by liquid scintillation counting: An evaluation of chemical quenching by liquid chromatographic eluents

The feasibility of utilizing liquid scintillation counting as a detection method for the liquid chromatographic analysis of⁹⁹Tc is evaluated. The chemical quenching of constituents commonly found in liquid chromatographic mobile phases is investigated, and quench corrections are presented. Quantification of⁹⁹Tc is achieved over a concentration range of 10^–3 to 10^–8M on quiescent KTCO₄ solutions, with sample volumes of 0.3 ml, yielding a counting efficiency from 51 to 59% for a narrow 150 channel window. The potential for the double isotope labelling of technetium complexes and the implications of the liquid scintillation counting of⁹⁹Tc in flowing eluents are discussed.     

A novel method for the simultaneous determination of125I and14C activities using liquid scintillation counting

The viability of a dual label liquid scintillation technique has been investigated. To avoid the need for two procedures, gamma counting for¹²⁵Iodine (¹²⁵I) and liquid scintillation counting for¹⁴C. Since the¹²⁵I spectrum covers almost as wide a range of pulse heights as¹⁴C, conventional dual label methods would result in very low¹⁴C counting efficiencies. The conventional dual label technique has ben modified to increase the¹⁴C counting efficiency and to accomodate the consequent additional spillover of¹²⁵I counts into the upper window. This dual label technique has been applied to the determination of¹²⁵I and¹⁴C activities in blood samples. The accuracy of the method has been tested, and its advantages and limitations are discussed.     

Precise trace rare earth analysis by radiochemical neutron activation

A rare earth group separation scheme followed by normal Ge(Li), low energy photon detector (LEPD), and Ge(Li)−NaI(Tl) coincidence-noncoincidence spectrometry significantly enhances the detection sensitivity of individual rare earth elements (REE) at or below the ppb level. Based on the selected γ-ray energies, normal Ge(Li) counting is favored for¹⁴⁰La,¹⁷⁰Tb and¹⁶⁹Yb; LEPD is favored for low γ-ray energies of¹⁴⁷Nd,¹⁵³Sm,¹⁶⁶Ho and¹⁶⁹Yb; and noncoincidence counting is favored for¹⁴¹Ce,¹⁴³Ce,¹⁴²Pr,¹⁵³Sm,¹⁷¹Er and¹⁷⁵Yb. The detection of radionuclides^152mEu,¹⁵⁹Gd and¹⁷⁷Lu is equally sensitive by normal Ge(Li) and noncoincidence counting;¹⁵²Eu is equally sensitive by LEPD and normal Ge(Li); and¹⁵³Gd and¹⁷⁰Tm is equally favored by all the counting modes. Overall, noncoincidence counting is favored for most of the REE. Precise measurements of the REE were made in geological and biological standards. Prepared for the U.S. Department of Energy under Contract DE-AC06-76RLO 1830.     

Possible overestimation of the external standard quench parameter on Wallac 1220 Quantulus™ with high energetic beta-emitters

The 1220 Quantulus is equipped with an ¹⁵²Eu external source used to determine an external standard quench parameter SQP(E). The relationship between ⁹⁰Sr/⁹⁰Y counting efficiency and SQP(E) was found linear in a defined range of SQP(E) values. This function was fixed after many counting experiences made with ⁹⁰Sr/⁹⁰Y standards. The sasme equation is used for the measurement of ⁹⁰Sr in environmental samples. The first goal of this paper is to objectify an overestimation of the SQP(E) when high energetic beta-emitters like ⁹⁰Y are present (1 to 4% in routine conditions). The second one is to show how this artefact could induce a bias in the calculation of ⁹⁰Sr activity in environmental samples. The median of this overestimation is estimated around 6%. Another approach using ⁸⁵Sr standard is suggested to avoid this overestimation. Provided the chemical composition — and thus the quenching — is similar for the two standards, the counting efficiency measured with the ⁹⁰Sr/⁹⁰Y standard could be related to the SQP(E) value of the ⁸⁵Sr standard. Indeed this one appears to be more robust regarding to the range of activity and to the counting time of the external source.     

Flow-through radioactivity detection of 3H- and 14C-labelled compounds in reversed-phase liquid chromatography by a liquid scintillation counting technique based on post-column extraction

A method for flow-through liquid scintillation counting in reversed-phase liquid chromatography (RP-LC) based on the continuous extraction of aqueous column eluates with a water-immiscible liquid scintillator is evaluated in terms of sensitivity, reproducibility and extra-column band broadening. ³H- and ¹⁴C-labelled phenylthiohydantoinamino acid derivatives of widely different polarity serve as model compounds. For extractable derivatives, counting efficiencies of over 30 and 80% can be obtained for ³H and ¹⁴C, respectively. The reproducibility and extra-column band broadening depend on the mixing ratio of scintillator and LC eluent; relative standard deviations (peak areas) of less than 3% can be obtained. The sensitivity of flow-through counting can be increased at least 150-fold by storing the segmented scintillator/eluate stream in a capillary storage loop. After the separation is complete, the stream is re-introduced into the radioactivity detector at reduced flow-rates to increase the mean residence time, i.e., the counting time, in the detector.     

Limit of the INAA procedure for copper determination based on the64Cu 511 keV line

The²³⁵U/²³⁸U ratio is determined by neutron activation analysis counting the ϕ-rays of short half-lives fission products and²³⁹U. The effect of the neutron spectrum hardening using a⁶LiD converter is also demonstrated. The²³⁵U/²³⁸U ratio is determined using short irradiation, waiting and counting times.     

Liquid scintillation counting of radionuclides emitting high-energy beta radiation

Liquid scintillation counting of radionuclides emitting beta radiation with E_max>2 MeV has been investigated. Fluor volume effects were similar to those for low energy beta radiation, and pulse height spectra broadened in a predictable manner with no pulse clipping up to 4.913 MeV. Large changes in sample channels ratio due to color quenching resulted in progressively smaller losses of counting efficiency as beta energy increased. Counting efficiences were estimated to be near 100 percent for³⁴Cl^m,³⁶Cl,³²P and³⁸Cl. Cerenkov counting of³⁸Cl by liquid scintillation counter was volume dependent for both counting efficiency and pulse height spectrum. Counting efficiencies for³⁴Cl^m,³⁶Cl,³²P and³⁸Cl were estimated to be 57.0, 7.5, 42.7 and 66.3%, respectively. Pulse height spectra were shifted to greater pulse heights as a function of beta E_max, supporting the possibility of energy discrimination for beta emitters by Cerenkov pulse height spectrum analysis. The advantage of singles Cerenkov counting over coincidence Cerenkov counting was greatest for³⁶Cl and least for³⁸Cl; this advantage was amplified more for samples of³⁶Cl which had been color quenched than for similarly quenched samples of³⁸Cl or³²P.     

Determination of uranium by thermal and epithermal neutron activation in natural waters and in human urine

Uranium is determined via its ²³⁹U nuclide (74.0 keV, t_{$\text{1}\text{2}$} = 23.5 min) in natural waters down to 0.03 ng U ml^-1 after preconcentration with activated carbon and oxine; 30-min irradiation and counting times are used. No preconcentration is required for samples containing more than 4 ng U ml^-1 with 10-min irradiation and counting times. Uranium in urine can be determined under a boron shield at the 5 ng ml^-1 level after 30-min irradiation and counting.     

Preconcentration and separation of <Superscript>99</Superscript>Tc in groundwater by using TEVA resin

An effort has been made to optimize the counting time for low-level measurement of naturally occurring radioactive material (NORM) by considering the standard deviation between the activity values of different photopeaks and counting error. It is observed that at lower counting time, relative standard deviation (RSD) varies randomly, but attains a gradual trend with increasing time and also comes closure to the counting error. Therefore minimum counting time for low-level NORM measurement of ²³⁸U and ²³²Th would be the time required to stabilize the RSD values.     

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.     

Low level determination of thallium in biological and environmental reference materials by RNAA using several counting methods

A new RNAA procedure was developed capable of low level determination of thallium in biological and environmental samples. After high fluence neutron irradiation in a nuclear reactor, wet ashing of samples and T1(I) separation by solvent extraction with sodium diethyldithiocarbamate at pH 13, several types of counting were employed to compare their detection limits and to utilize the self-validation principle of NAA. The following measurement modes were used: High efficiency counting of -rays of²⁰²T1 and Hg X-rays produced on decay of²⁰⁴T1 using a well-type HPGe detector, combined ^– ray and ^–-counting of²⁰⁴T1 with the aid of a HPGe planar detector, and liquid scintillation counting and counting of Cerenkov radiation of ^–-particles of²⁰⁴T1. The lowest detection limit of 0.034 ng of T1 was achieved on liquid scintillation counting of²⁰⁴T1. The method was applied for the analysis of biological NIST SRMs 1515, 1573a, 1577b and environmental NIST SRM 1633a. Good agreement was found between the thallium certified value in SRM 1633a and values determined in this work by all counting modes. For SRM 1573a, results in agreement were obtained by two counting modes, while counting of Hg X-rays of²⁰⁴T1 was only used for SRMs 1515 and 1577b.     

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.