Advantages of low-background liquid scintillation alpha-spectrometry and pulse shape analysis in measuring222Rn, uranium and226Ra in groundwater samples

Liquid scintillation counting (LSC) and pulse shape analysis (PSA) was used in measuring radon and gross alpha- and beta-activities in groundwater. We used conventional LSC counters for the measurement of radon in water, but low-background LSC spectrometers for the gross activity measurements. The lower limit of detection (LLD) for radon in water is 0.6 Bq/l for a 60 min count with a conventional counter, but 0.1 or 0.2 Bq/l, with the two types of low-background LSC spectrometers equipped with a pulse shape analyser (PSA). The gross alpha and beta activity measurements are made using a simple sample preparation method, PSA of a low background LSC and spectrum analysis. The LLD recorded for gross alpha and beta with the two spectrometers are 0.02 and 0.03 Bq/l and 0.2 and 0.4 Bq/l, respectively, for a 180 minutes count and a 38 ml sample volume. The method also enable the calculation of the U and²²⁶Ra contents in water and indicates the presence of some other long-lived radionuclides (²¹⁰Pb,²²⁸Ra or⁴⁰K). The LLD for U recorded with both spectrometers is 0.02 Bq^–1 and for²²⁶Ra 0.01 Bq·1^–1. The LLDs attained by this LSC method are two orders of magnitude lower than the maximum permissible concentrations set for U and²²⁶Ra.     

A Portable Liquid Scintillation Counter for General LSC and High Sensitivity Alpha-Counting Applications

Applicability of a new portable, single tube liquid scintillation (LS) spectrometer was demonstrated for general LS applications, such as wipe tests and low level alpha counting, especially radon (²²²Rn) measurements in water. Wipe tests were performed with wad sticks. They were counted conventionally in a small volume in Eppendorf tubes with less than 200µl of LS cocktail, thus minimizing costs and waste. Small volume is specially recommended because low background can be achieved without heavy lead shielding, thus maintaining portability. Typical NRC recommended LLD's were reached for ³H and other typical LS isotopes. For ²²²Rn in water a biphasic extraction system was adopted where radon is extracted from water into a water-immiscible LS cocktail. The method is sensitive because radon can be extracted from a large water volume. It was observed that common non-evaporating "safe" cocktails with di-isopropyl naphtalene solvent are convenient to use and quite suitable for extraction. Also the isotope ²²⁶Ra can be reliably measured via production of its daughter ²²²Rn. The instrument includes pulse shape electronics to perform alpha/beta separation. This is based on the fact that in LS cocktails alphas generate pulses with longer duration than betas. The alpha/beta separation can be visualized with a two dimensional graph where the x-axis represents pulse amplitude (MCA channels) and the y-axis its length. The graphical operations are all done in standard Excel/Windows environment. Due to their longer pulses, alphas have greater y-coordinates than betas with the same x-coordinate (amplitude). With this graph, one can select a region occupied only by alphas and exclude betas. The above mentioned "safe" cocktails posses good alpha/beta separation properties. Because natural background (cosmic-rays and environmental gammas) produces beta-like pulses, they can be stripped away giving low background for alpha counting, typically a few counts per hour for the extraction samples. The LLD for ²²²Rn was 0.1 Bq/I.     

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.     

Study of Long-Term Radon Progeny in Humans for Retrospective Evaluation of Radon Exposure

An individual in vivo monitor using seven Germanium detectors with a total area of 24,000 mm² was prepared for ²¹⁰Pb skull measurements. System calibration with anthropomorphic head phantoms and a straightforward efficiency estimation yielded a minimum detectable activity (MDA) of 6.7 Bq and a lower limit of detection (LLD) of 14 Bq (CL: 95%). Two selected persons were measured for 1 h each to reconstruct their cumulative radon exposure. From the added pulse height spectrum a ²¹⁰Pb activity in the skull of 3.1±7.2 Bq (result with 95%-CL) was estimated, but clear conclusions on their radon exposure using a new metabolism model of lead in man could not be drawn. Further improvements in the selection of highly exposed persons as well as head calibration and Lackground reduction are necessary using this attempt for retrospective exposure reconstruction.     

Evaluating the potential alpha energy of radon progeny

Potential alpha energy concentration of radon progeny can be measured using the alpha-spectroscopy with the silicon semiconductors detectors and the gross-counting attached with the ZnS detectors. The decay method was applied where the alpha particles emitted from the ²¹⁸Po to ²¹⁴Po were detected. In the case of the decay products, the amount and aerodynamic behavior of radioactivity are important, and also need to be measured. During the experiment, the radon gas was supplied and evaluated from the experimental room with constant concentration. Then the air sample was used as the known volume and the grab sampling technique was developed for estimating the concentration of radon decay products. However the proper calculation was applied for estimating the potential alpha energy of radon progeny through of ²¹⁸Po, ²¹⁴Pb and ²¹⁴Bi.     

Measurement of radon in air by α track method enhancement of detection sensitivity using a lamp

A new α track method is proposed for the measurement of radon (²²²Rn) concentration in environmental levels. This involves collecting radon daughters on the surface of pilot lamp and detecting α-particles emitted from the nuclides (²¹⁸Po and²¹⁴Po) by a detector (LR 115). The detection sensitivity of this method is 6 times greater than that of the conventional α track method.     

Determination of atmospheric lead-210 by alpha-scintillation counting of air filters

Alpha-counting of filters used to sample large volumes of air provides a convenient way of determining atmospheric concentrations of²¹⁰Pb. Following decay of short-lived²²²Rn and²²⁰Rn progeny, alpha activity of the filters increases as²¹⁰Pb decays to²¹⁰Po. After transient equilibrium is reached at about 3 y, alpha activity diminishes with the 22.3 y halflife of²¹⁰Pb. The degree of equilibrium between²¹⁰Pb and²¹⁰Po can be calculated subsequent to sampling, and the average concentration of²¹⁰Pb in the air during the sampling period can be computed. Contributions to the total²¹⁰Pb from ambient short-lived radon progeny are small, typically 2–4%. Using high volume air samplers with collection rates of 1.1–1.7 m³/min for 24 h periods, and using counting times of 2 h for 20 cm² filter sections, we measured alpha counts ranging from 0.0100±0.0050 to 0.200±0.0200 dps. Periodic measurements on 100 of these filters over a 4 y period yielded mean²¹⁰Pb levels with standard deviations less than ±15%. The method requires minimal sample preparation and can be used to determine past atmospheric²¹⁰Pb concentrations on filters stored for up to 20 y and more.     

Development of a method for the determination of 226Ra by liquid scintillation counting

Liquid scintillation counting has not been widely applied to a-particle detection because of its poor energy resolution and variable background. In the present work, a time saving and reasonably accurate method for determination of ²²⁶Ra in water has been developed, using liquid scintillation spectrometry and pulse-shape analysis. The effect of three levels of chemical quench on the spillover of alpha interactions into the beta window and vice versa was assessed. The advantages of liquid scintillation in comparison with other methods (radon emanation) for determination of ²²⁶Ra are the high counting efficiency (~100%) and the easier sample preparation, with no need for sample preconcentration.     

Concentrations of radon,thoron and their decay products measured in natural caves and ancient mines by using solid state nuclear track detectors and resulting radiation dose to the members of the public

Alpha- and beta-activities per unit volume of air due to radon (²²²Rn), thoron (²²⁰Rn) and their progenies were measured in the air of natural caves and ancient mines as well as inside different reference atmospheres by using CR-39 and LR-115 type II solid state nuclear track detectors (SSNTDs). In addition, the radon concentration was continuously measured inside one of the studied caves by using the SSNTDs’ method and AlphaGuard counter. Equilibrium factors between radon and its daughters and between thoron and its progeny were evaluated in the studied atmospheres. Alpha-activities due to ²¹⁸Po and ²¹⁴Po short-lived radon decay products were determined in different compartments of the respiratory tract of members of the public. The committed equivalent doses due to the ²¹⁸Po and ²¹⁴Po radon short-lived progeny were evaluated in different tissues of the respiratory tract of the visitors of the considered caves and ancient mines. Annual effective doses due to radon progeny from the inhalation of air by the visitors of the studied caves and ancient mines were evaluated.     

Determination of 210Po in Reagent Samples by Alpha-Ray Spectrometry Using Extraction Chromatographic Resin

The determination of ²¹⁰Po in phosphoric acid reagent by alpha-ray spectrometry using extraction chromatographic resin is presented. The decontamination factors of interference elements were measured. It was observed that HCl, HNO₃, ascorbic acid, thioacetamide and Cu were free from ²¹⁰Po but Pb contain small amounts of ²¹⁰Po. ²¹⁰Po in phosphoric acid samples was ranged from <8 to 2.4 Bq/l. The detection limit of ²¹⁰Po in 50 ml of phosphoric acid is 8 mBq/l with a counting time of 1 day undercounting efficiency of 30%.     

Determination of polonium-210 in phosphoric acid

Polonium-210 in phosphoric acid has been recognized as a significant source of alpha contamination of processed Si-wafers for memory devices of computer. In the present work, a convenient method was developed for the determination of trace²¹⁰Po in phosphoric acid of high purity. For the determination,²⁰⁹Po was used as a yield tracer. The present method consists of (1) addition of the tracer to 5 ml aliquot of phosphoric acid sample, (2) pH adjustment (to 2) of the sample solution to make up electrolytic solution, (3) electrodeposition for the simultaneous achievement of Po separation and preparation of counting source on stainless-steel disc, and (4) alpha-ray spectrometry. By the developed method, more than 95% of Po was separated from phosphoric acid sample onto counting disc. The minimum detectable radioactivity of²¹⁰Po in 5 ml of phosphoric acid was about 0.03 mBq by counting the electrodeposited alpha-activity for 10 days under a counting efficiency of ≈30%.     

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.     

An assessment of the selection criteria for an analytical method for radium-226 in environmental samples

This paper examines the process of making a decision on the optimum technique for the measurement of low concentrations of²²⁶Ra in environmental materials. The available counting techniques are alpha spectrometry, high resolution gamma spectrometry and liquid scintillation counting. The properties of the analytical technique; sensitivity, lower limit of detection (LLD) and precision are considered. Method selection is also restricted by the available sample size and activity. The influence of procedure backgrounds, geometric efficiency, chemical recovery, counting time, sample size and activity on the precision and LLD are investigated. The process of method selection, applicable to a wide range of samples, is illustrated by reference to sediments, waters and tissues.     

A case study on the effect of water from groundwater sources on indoor radon levels

Indoor airborne radon concentration released from water was estimated over several months based on experimental measurements. When heated water including radon was used, the radon level became high in the entire house. Filling the bathtub with hot water had a strong effect on the indoor radon level. In winter, the indoor radon concentration was high due to windows being closed. The radon transfer coefficient was estimated 2.5·10⁻⁴ in this test house. This is 2.5 times higher than the average radon transfer efficiency estimated by UNSCEAR.     

Field measurement of the <Superscript>218</Superscript>Po, <Superscript>214</Superscript>Pb and <Superscript>214</Superscript>Bi concentrations in typical indoor and outdoor environments in Beijing

The activity concentrations of ²¹⁸Po, ²¹⁴Pb and ²¹⁴Bi [i.e. C(²¹⁸Po), C(²¹⁴Pb), and C(²¹⁴Bi)] and the calculated concentration ratios [i.e. 1:C(²¹⁴Pb)/C(²¹⁸Po):C(²¹⁴Bi)/C(²¹⁸Po)] are necessary for assessing radon and its progenies exposure. In this study, a measurement method of radon progenies concentrations with both high sensitivity and low uncertainty, was developed based on the Kerr method. The field measurement results of radon progeny concentrations and calculated concentration ratios in both typical indoor and outdoor environments in Beijing, China, were reported. The effects of air exchange rate on concentration ratios of radon progenies in indoor environments were discussed.     

Field alpha-spectroscopy of radon (<Superscript>222</Superscript>Rn) and actinon (<Superscript>219</Superscript>Rn) progeny in soil gas: Locating a radon source

Summary The activities of²¹⁸Po,²¹⁴Po and²¹¹Bi were determined in samples obtained of soil/gas. Sampling work was taken in Jáchymov (Czech Republic) at the outcrop of the Geister-vein,by electrostatic precipitation from filtered soil gas on stainless steel disks.The samples were measured in a field laboratory using a semi-conductor alpha-spectrometer.The activities of²¹⁸Po,²¹⁴Po and²¹¹Bi were calculated.Samples taken from active dump material (near-by radon source) exhibited a high²¹¹Bi/²¹⁴Po ratio, while those of the vein outcrop (a relatively deeper source) had a low ratio.A mathematical model was employed to determine the radon age calculated from the actinon/radon input ratio.This varied in a range of 5.6 to -7.7 seconds.Negative age values are probably caused by the preference for actinon, which rapidly comes into equilibrium with the source of this gas.     

Optimization of liquid scintillation counting techniques for the determination of carbon-14 in environmental samples

The goal of this work was to optimize the liquid scintillation counting techniques for the determination of¹⁴C in stack effluent gases and in environmental samples such as biological and air samples. Carbon-14 activities in most environmental samples were measured with the direct CO₂ absorption method. The highest figures of merit were found through the variation of Carbosorb E and Permafluor V ratio, and measurement windows. The best condition was an 1:1 volume ratio. Average 2.35 g of CO₂ was reproducibly absorbed in the 20 ml mixture within 40 minutes. The counting efficiency determined by repeated analysis of NIST oxalic acid standard and the background count rate were measured to be 58.8±1.4% and 1.88±0.06 cpm, respectively, in case of saturated solution. The correction curves of counting efficiency for partially saturated solutions and for saturated solutions with quenching were prepared, respectively. The overall uncertainty of the sample specific activity for near background levels was estimated to be about 7% for 4 hours counting at 95% confidence level. Stack effluent gas samples were measured by a gel suspension counting method. After precipitation of CO₂ in the form of BaCO₃, 140 mg of which was mixed with 6 ml H₂O and 12 ml of Instagel XF. The counting efficiency was measured to be 71.5±1.7% and the typical sensitivity of this technique was about 510 mBq/m³ for a 100 min count at a background count rate of 4.7 cpm. For the benzene counting method measurements were performed with a mixture of 3 ml benzene and 1 ml of scintillation cocktail (5 g of butyl-PBD in 100 ml of scintillation-grade toluene) in a low potassium 7 ml borosilicate glass vial. The counting efficiency and the background count rate were measured to be 64.3±1.0% and 0.51±0.05 cpm, respectively. The long-term stability of samples has been checked for all the counting techniques over a two week period, during which no apparent change in counting efficiency and background level was found.     

Determination of <Superscript>228</Superscript>Ra in human bone ash containing significant quantities of <Superscript>40</Superscript>K and Ca<Superscript>2+</Superscript>

The determination of ²²⁸Ra by means of γ-spectrometry, in material containing significant quantities of ⁴⁰K and Ca²⁺ such as bone ash results in increased values of counting uncertainty and lower limit of detection (LLD) because of a significant contribution from the Compton continuum of ⁴⁰K. However, ⁴⁰K is widely removed from bone ash if ²²⁸Ra is coprecipitated with barium sulfate. As a result, the counting uncertainty and LLD are significantly reduced. A method is presented for determination of very low activity concentrations of ²²⁸Ra. Impurities introduced by precipitation are negligible when applying high resolution γ-spectrometry.     

Radioactivity mapping of north western areas of Pakistan

Summary A systematic study of natural and fall-out radionuclides was carried out with the environmental samples of soil, vegetation and water from some regions of North West Frontier Province (NWFP) of Pakistan. The pretreatment of the samples was performed in the laboratory using IAEA recommended methods. The analysis of gamma-emitters such as ⁴⁰K, ²²⁶Ra, ²³² Th and ¹³⁷Cs was performed with a high purity germanium detector (HPGe). For the determination of ⁹⁰Sr, a liquid scintillation counting system was used. The average specific activities of ⁴⁰K, ²²⁶Ra, ²³² Th and ¹³⁷Cs have been found to be 307±101 Bq ^. kg^-1, 10.2±3 Bq ^. kg^-1, 24±6 Bq ^. kg^-1 and 2.8±1.3 Bq ^. kg^-1, respectively, in soil samples. Vegetation samples have smaller values of specific activities and even the analysis of water samples showed values less than LLD for earlier reported radionuclides. Other parameters like hazard indices, radium equivalent activities, absorbed dose rates and effective dose equivalents have also been determined. All these parameters have values less than their respective limiting values representing that the surveyed areas have no significant hazard from health point of view. Analysis of ⁹⁰Sr for all the samples showed results below LLD. The present study provides a general background of the detectable radionuclides for the surveyed areas that will be helpful in any radiological emergency.     

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.