Measurement and modelling of radioxenon plumes in the Ottawa Valley

Since 2001 a real-time radiation monitoring network of Canadian nuclear facilities and major population centres has been implemented for response to nuclear incidents including a possible terrorist attack. Unshielded NaI(Tl) spectroscopic detectors are employed to measure gamma radiation from airborne radioactivity and radioactivity deposited on the ground. These detectors are composed of a standard 3'x3' cylindrical NaI(Tl) spectrometers with data storage and integrated telemetry. Some of the detectors have been deployed in the Ottawa Valley near Chalk River Laboratories and Ottawa, which has a complex radioxenon environment due to the proximity of nuclear power reactors, and medical isotope facilities. Although not a health threat, these releases have provided an opportunity for the Canadian Meteorological Centre and the Commissariat à l'Energie Atomique to validate their meteorological models. The meteorological models of the two organizations are in good agreement on the origin and the source terms of these releases.     

The influence on the radioxenon background during the temporary suspension of operations of three major medical isotope production facilities in the Northern Hemisphere and during the start-up of another facility in the Southern Hemisphere

Medical isotope production facilities (MIPF) have recently been identified to emit the major part of the environmental radioxenon measured at many globally distributed monitoring sites deployed to strengthen the radionuclide component of the Comprehensive Nuclear-Test-Ban Treaty (CTBT) verification regime. Efforts to raise a global radioxenon emission inventory revealed that the yearly global total emission from MIPF’s is around 15 times higher than the total radioxenon emission from nuclear power plants (NPP's).Given that situation, from mid 2008 until early 2009 two out of the ordinary hemisphere-specific events occured:1) In the Northern hemisphere, a joint temporary suspension of operations of the three largest MIPF's made it possible to quantify the effects of the emissions related to NPP’s. The average activity concentrations of ¹³³Xe measured at a monitoring station close to Freiburg, Germany, went down significantly from 4.5 ± 0.5 mBq/m³ to 1.1 ± 0.1 mBq/m³ and in Stockholm, Sweden, from 2.0 ± 0.4 mBq/m³ to 1.05 ± 0.15 mBq/m³.2) In the Southern hemisphere the only radioxenon-emitting MIPF in Australia started up test production in late November 2008. During eight test runs, up to 6.2 ± 0.2 mBq/m³ of ¹³³Xe was measured at the station in Melbourne, 700 km south-west from the facility, where no radioxenon had been observed before, originating from the isotopic production process.This paper clearly confirms the hypothesis that medical isotope production facility are at present the major emitters of radioxenon to the atmosphere. Suspension of operations of these facilities indicates the scale of their normal contribution to the European radioxenon background, which decreased two to four fold. This also gives a unique opportunity to detect and investigate the influence of other local and long distance sources on the radioxenon background. Finally the opposing effect was studied: the contribution of the start-up of a renewed radiopharmaceutical facility to the build up of a radioxenon background across Australia and the Southern hemisphere.     

Detection and analysis of xenon isotopes for the comprehensive nuclear-test-ban treaty international monitoring system

The use of the xenon isotopes for detection of nuclear explosions is of great interest for monitoring compliance with the comprehensive nuclear-test-ban treaty (CTBT). Recently, the automated radioxenon sampler-analyzer (ARSA) was tested at the Institute for Atmospheric Radioactivity (IAR) in Freiburg, Germany to ascertain its use for the CTBT by comparing its results to laboratory-based analyses, determining its detection sensitivity and analyzing its results in light of historical xenon isotope levels and known reactor operations in the area. Xe-133 was detected nearly every day throughout the test at activity concentrations ranging between approximately 0.1 mBq/m3 to as high as 120 mBq/m3. Xe-133m and 135Xe were also detected occasionally during the test at concentrations of less than 1 to a few mBq/m3.     

Global radioxenon emission inventory based on nuclear power reactor reports

Atmospheric radioactivity is monitored for the verification of the Comprehensive Nuclear-Test-Ban Treaty, with xenon isotopes ^131mXe, ¹³³Xe, ^133mXe and ¹³⁵Xe serving as important indicators of nuclear explosions. The treaty-relevant interpretation of atmospheric concentrations of radioxenon is enhanced by quantifying radioxenon emissions released from civilian facilities. This paper presents the first global radioxenon emission inventory for nuclear power plants, based on North American and European emission reports for the years 1995–2005. Estimations were made for all power plant sites for which emission data were unavailable. According to this inventory, a total of 1.3 PBq of radioxenon isotopes are released by nuclear power plants as continuous or pulsed emissions in a generic year.     

Machine learning for radioxenon event classification for the Comprehensive Nuclear-Test-Ban Treaty

A method of weapon detection for the Comprehensive nuclear-Test-Ban-Treaty (CTBT) consists of monitoring the amount of radioxenon in the atmosphere by measuring and sampling the activity concentration of ^131mXe, ¹³³Xe, ^133mXe, and ¹³⁵Xe by radionuclide monitoring. Several explosion samples were simulated based on real data since the measured data of this type is quite rare. These data sets consisted of different circumstances of a nuclear explosion, and are used as training data sets to establish an effective classification model employing state-of-the-art technologies in machine learning. A study was conducted involving classic induction algorithms in machine learning including Naïve Bayes, Neural Networks, Decision Trees, k-Nearest Neighbors, and Support Vector Machines, that revealed that they can successfully be used in this practical application. In particular, our studies show that many induction algorithms in machine learning outperform a simple linear discriminator when a signal is found in a high radioxenon background environment.     

The influence of radiopharmaceutical isotope production on the global radioxenon background

Radioxenon isotopes play a major role in confirming whether or not an underground explosion was nuclear in nature. It is then of key importance to understand the sources of environmental radioxenon to be able to distinguish them from those of a nuclear explosion.     

Geochemical estimation of copper contamination in the healing mud from Makirina Bay, central Adriatic

The coastal sediment from Makirina Bay in the central Adriatic represents an important source of healing mud (peloid) of high quality organoleptic properties that could in future be used for medical treatment. In this study, we estimated the contamination of the sediment with copper which can cause some undesirable health effects. Concentrations of Cu vary from 12 to 63 mg/kg in surface sediment and are higher in the central part of the Bay where the mud fraction prevails. Different normalizing methods were used, i.e. surface/background ratio, index of geoaccumulation, reference metal normalization, enrichment factor (EF) and grain size normalization, to compensate for the influence of the natural variability in sediment mineralogy and granulometry, and to assess whether the concentrations observed in surface sediment represent background or contaminated levels. Results show that Cu concentrations in the surface sediment are twice as high as local background values but in the same range as many clay materials used for medical treatment in Italy. The results also show that more detailed studies on Cu mobility are necessary prior to actual use of peloid in medical treatment.     

Radioactivity level and soil radon measurement of a volcanic area in Cameroon

The radioactivity level of soils in a volcanic area in Cameroon was determined and discussed. Thirty soils samples were collected from Buea and Limbé cities located in the south-western Cameroon. These two regions are known for theirs volcanic grounds due to the presence of Mount Cameroon Mountain. The activity concentrations of natural radionuclides as well as that of the fission product were evaluated by gamma-ray spectrometry using a hyper-purity germanium detector (HPGe). The ranges of concentrations in the surveyed soils were 11-17 Bq kg(-1), 22-36 Bq kg(-1) and 43-201 Bq kg(-1) for (226)Ra, (232)Th and (40)K, respectively. The radioisotope (137)Cs was also found but in a very small amount. The outdoor absorbed dose rate 1m above ground with the corresponding annual effective dose rate, assuming a 20% occupancy factor was estimated. The radium equivalent and the external hazard index were also evaluated and results are compared with available data from other studies and with the world average value [United Nations Scientific Committee on the Effects of Atomic Radiation (UNSCEAR), 1988. Sources, Effects and Risks of Ionizing Radiation. Report to the General Assembly on the Effects of Atomic Radiation. United Nations, New York; UNSCEAR, 2000. Sources and Effects of Ionizing Radiations. Report to the General Assembly with Scientific Annexes. United Nations, New York]. A solid state nuclear track detector (SSNTD), LR-115 was used for soil radon measurements at a depth of 50 cm. The ranges of soil radon concentrations were 6.7-10.8 kBq m(-3) and 5.5-8.7 kBq m(-3) in Buea and Limbé, respectively. A positive correlation was found between concentrations of radium measured with gamma-spectrometry and the soil radon concentrations measured with the nitrate cellulose detectors. The results of this study provide the radioactivity level in soil of a volcanic area, which has been found to be within the safety limits. The south-western Cameroon can be considered as having normal natural background radiation.     

Primordial radionuclides in Canadian background sites: secular equilibrium and isotopic differences

A literature review and field sampling were done to obtain information on primordial (natural-series) radionuclide concentrations in terrestrial environments in diverse locations across Canada. Of special interest was the degree of secular equilibrium among members of decay series. The analytes measured in soils and plants were (nat)U by neutron activation-delayed neutron counting, (228)Th, (230)Th, (232)Th, (226)Ra and (210)Po by alpha spectroscopy, (210)Pb by gas flow proportional counting, (228)Ra by beta counting and (137)Cs by gamma spectroscopy. In addition, ICP-MS was used to obtain concentrations of about 50 analytes including elemental U, Pb, and Th. Samples were from seven representative background sites with a total of 162 plant samples from 38 different species. These data were supplemented by a review that gathered a large portion of the similar data from published sources. The sites chosen were semi-natural, far from any nuclear industry, although several were specifically located in areas with slightly elevated natural U concentrations. As might be expected, there were many cases of non-detectable concentrations. However, certain trends were evident. The activity ratio (210)Po/(210)Pb was unity in soils and non-annual plant tissues such as lichens. It was about 0.6 in annual plant tissues. These results are consistent with the time required for ingrowth of (210)Po to reach secular equilibrium. There was evidence from several sources that (210)Pb in plants came predominantly from deposition of (210)Pb from air after the decay of airborne (222)Rn. This was expected. Somewhat unexpected was the observation that (228)Th seemed to be much more plant available than (232)Th, even though both are in the same decay series and should be chemically similar. The difference was attributed to the combined effects of ingrowth from (228)Ra in the plant and effects of alpha recoil in mobilizing (228)Th in the soil. In general, the results of this study will benefit risk assessment, both in providing background concentrations, but also some indication of where isotope activity ratios can and cannot be used to estimate concentrations.     

Numerical simulation of 137Cs and (239,240)Pu concentrations by an ocean general circulation model

We simulated the spatial distributions and the temporal variations of 137Cs and (239,240)Pu concentrations in the ocean by using the ocean general circulation model which was developed by National Center of Atmospheric Research. These nuclides are introduced into seawaters from global fallout due to atmospheric nuclear weapons tests. The distribution of radioactive deposition on the world ocean is estimated from global precipitation data and observed values of annual deposition of radionuclides at the Meteorological Research Institute in Japan and several observed points in New Zealand. Radionuclides from global fallout have been transported by advection, diffusion and scavenging, and this concentration reduces by radioactive decay in the ocean. We verified the results of the model calculations by comparing simulated values of 137Cs and (239,240)Pu in seawater with the observed values included in the Historical Artificial Radionuclides in the HAM database, which has been constructed by the Meteorological Research Institute. The vertical distributions of the calculated 137Cs concentrations were in good agreement and are in good agreement with the observed profiles in the 1960s up to 250 m, in the 1970s up to 500 m, in the 1980s up to 750 m and in the 1990s up to 750 m. However, the calculated 137Cs concentrations were underestimated compared with the observed 137Cs at the deeper layer. This may suggest other transport processes of 137Cs to deep waters. The horizontal distributions of 137Cs concentrations in surface water could be simulated. A numerical tracer release experiment was performed to explain the horizontal distribution pattern. A maximum (239,240)Pu concentration layer occurs at an intermediate depth for both observed and calculated values, which is formed by particle scavenging. The horizontal distributions of the calculated (239,240)Pu concentrations in surface water could be simulated by considering the scavenging effect.     

Distribution and sources of (129)I in rivers of the Baltic region

The concentration of (129)I was measured in 54 river waters discharging into the Baltic Sea from Sweden, Finland, Estonia, Latvia, Lithuania, Poland and Germany. Sample collection was performed during a well-bracketed time interval (June-July 1999), thus allowing comparison of the rivers over a wide latitude range without the effect of long temporal spread. Although there is no direct input of anthropogenic (129)I in the watersheds, the concentration of the isotope is about two to three orders of magnitude higher than the expected pre-nuclear era natural values in the rivers of Finland and northern Sweden, and in the rivers of southern Sweden, Lithuania, Estonia, Latvia, Poland and Germany; the (129)I concentration may reach five orders of magnitude higher. Furthermore, there are significant correlations between the (129)I concentration and latitude and/or distance from the North Sea and between (129)I and Cl. These findings suggest seawater as a main source of (129)I to the rivers through atmospheric transport. Of the many chemical parameters investigated, the pH may account for some of the variability in (129)I concentrations of the rivers. The contribution from nuclear weapon tests and the Chernobyl accident to the riverine (129)I is insignificant compared to the releases from the nuclear fuel reprocessing facilities. The total flux of (129)I by rivers to the Baltic Sea and related basins represents minor amounts of the isotope pool in these marine waters. External radioactivity hazards from (129)I are considered to be negligible in the Baltic region. However, as the main (129)I intake to the human body is likely through water, due to the large amount of daily water consumption, more concern should be given to internal radioactivity hazard that may be associated with the isotope's localized elevated concentration in the human organs.     

Domestic radon remediation of UK dwellings by Sub-Slab Depressurisation: evidence for a baseline contribution from constructional materials

To quantify the effectiveness of Sub-Slab Depressurisation, widely used in the United Kingdom (U.K.) to mitigate indoor radon gas levels in residential properties, a study was made of radon concentration data collected from a set of 170 homes situated in Radon Affected Areas in Northamptonshire and neighbouring counties, remediated using conventional sump/pump technology. A high incidence of satisfactory remediation outcomes was achieved, with 100% of the houses remediated demonstrating post-remediation radon concentrations below the U.K. domestic Action Level of 200 Bq m(-3), while more than 75% of the sample exhibited radon mitigation factors (defined as the ratio of radon concentrations following and prior to remediation) <0.2. Two systematic trends are identified. Firstly, absolute radon concentration reduction following remediation is directly proportional to initial radon concentration, with a mean reduction factor of 0.96 and a residual component of around 75 Bq m(-3). Secondly, houses with lower initial radon concentrations demonstrate poorer (higher) mitigation factors. These observations support a model in which the total indoor radon concentration within a dwelling can be represented by two principal components, one susceptible to mitigation by sub-slab depressurisation, the other remaining essentially unaffected. The first component can be identified with radon emanating from the subsoil and bedrock geologies, percolating through the foundations of the dwelling as a component of the soil-gas, and potentially capable of being attenuated by sub-slab depressurisation or radon-barrier remediation technologies. The second contribution can be identified with radon emanating from materials used in the construction of the dwelling with a further contribution from the natural background level, and is essentially unaffected by ground-level remediation strategies. Modelling of a multi-component radon dependency using ground-radon attenuation factors derived from the experimental data, in conjunction with typical background and structural-radon levels, yields behaviour in good agreement with the observed dependence of mitigation factor on initial radon concentration.     

Measurements and analysis of criteria pollutants in New Delhi, India

Ambient concentrations of carbon monoxide (CO), nitrogen oxides (NOx), sulfur dioxide (SO2), and total suspended particulates (TSP) were measured from January 1997 to November 1998 in the center of downtown [the Income Tax Office (ITO) located on B.S.G. Marg] New Delhi, India. The data consist of 24-h averages of SO2, NOx, and TSP as well as 8 and 24-h averages of CO. The measurements were made in an effort to characterize air pollution in the urban environment of New Delhi and assist in the development of an air quality index. The yearly average CO, NOx, SO2, and TSP concentrations for 1997 and 1998 were found to be 4810+/-2287 and 5772+/-2116 microg/m3, 83+/-35 and 64+/-22 microg/m3, 20+/-8 and 23+/-7 microg/m3, and 409+/-110 and 365+/-100 microg/m3, respectively. In general, the maximum CO, SO2, NOx, and TSP values occurred during the winter with minimum values occurring during the summer, which can be attributed to a combination of meteorological conditions and photochemical activity in the region. The ratio of CO/NOx (approximately 50) indicates that mobile sources are the predominant contributors for these two compounds in the urban air pollution problem in New Delhi. The ratio of SO2/NOx (approximately 0.6) indicates that point sources are contributing to SO2 pollution in the city. The averaged background CO concentrations in New Delhi were also calculated (approximately 1939 microg/m3) which exceed those for Eastern USA (approximately 500 microg/m3). Further, all measured concentrations exceeded the US National Ambient Air Quality Standards (NAAQS) except for SO2. TSP was identified as exceeding the standard on the most frequent basis.     

Spatial and time variations of radon-222 concentration in the atmosphere of a dead-end horizontal tunnel

The concentration of radon-222 has been monitored since 1995 in the atmosphere of a 2 m transverse dimension, 128 m long, dead-end horizontal tunnel located in the French Alps, at an altitude of 1600 m. Most of the time, the radon concentration is stable, with an average value ranging from 200 Bq m(-3) near the entrance to about 1000 Bq m(-3) in the most confined section, with an equilibrium factor between radon and its short-lived decay products varying from 0.61 to 0.78. However, radon bursts are repeatedly observed, with amplitudes reaching up to 36 x 10(3) Bq m(-3) and durations varying from one to several weeks, with similar spatial variations along the tunnel as the background concentration. These spatial variations are qualitatively interpreted in terms of natural ventilation. Comparing the radon background concentration with the measured radon exhalation flux at the wall yields an estimate of 8+/-2 x 10(-6) s(-1) (0.03+/-0.007 h(-1)) for the ventilation rate. The hypothesis that the bursts could be due to transient changes in ventilation can be ruled out. Thus, the bursts are the results of transient increased radon exhalation at the walls, that could be due to meteorological effects or possibly combined hydrological and mechanical forcing associated with the water level variations of the nearby Roselend reservoir lake. Such studies are of interest for radiation protection in poorly ventilated underground settings, and, ultimately, for a better understanding of radon exhalation associated with tectonic or volcanic processes.     

Radiostrontium hot spot in the Russian Arctic: ground surface contamination by (90)Sr at the "Kraton-3" underground nuclear explosion site

Strontium-90 activity concentrations in surface soils and areal deposition densities have been studied at a site contaminated by an accidental release to atmosphere from the underground nuclear explosion "Kraton-3" conducted near the Polar Circle (65.9 degrees N, 112.3 degrees E) within the territory of the former USSR in 1978. In 2001-2002, the ground surface contamination at 14 plots studied ranged from 20 to 15 000 kBq m(-2), which significantly exceeds the value of 0.44 kBq m(-2) deduced for three background plots. The zone with substantial radiostrontium contamination extends, at least, 2.5 km in a north-easterly direction from the borehole. The average (137)Cs/(90)Sr ratio in the ground contamination originated from the "Kraton-3" fallout was estimated to be 0.55, which is significantly different from the ratio of 2.05 evaluated for background plots contaminated mostly from global fallout. Although vertical migration of (90)Sr in all undisturbed soil profiles studied is more rapid than that for (137)Cs, the depth of percolation of both radionuclides into the ground is mostly limited to the top 10-20 cm, which may be explained, primarily, by permafrost conditions. The horizontal migration rate of radiostrontium in the aqueous phase exceeds the radiocaesium migration rate by many times. This phenomenon seems to be a reason for the significant enrichment of the soil surface layers by radiostrontium at some sites, with variations occurring in accordance with small-scale irregularities of landscape.     

Evaluation of radioxenon releases in Australia using atmospheric dispersion modelling tools

The origin of a series of atmospheric radioxenon events detected at the Comprehensive Test Ban Treaty Organisation (CTBTO) International Monitoring System site in Melbourne, Australia, between November 2008 and February 2009 was investigated. Backward tracking analyses indicated that the events were consistent with releases associated with hot commission testing of the Australian Nuclear Science Technology Organisation (ANSTO) radiopharmaceutical production facility in Sydney, Australia. Forward dispersion analyses were used to estimate release magnitudes and transport times. The estimated ¹³³Xe release magnitude of the largest event (between 0.2 and 34 TBq over a 2 d window), was in close agreement with the stack emission releases estimated by the facility for this time period (between 0.5 and 2 TBq). Modelling of irradiation conditions and theoretical radioxenon emission rates were undertaken and provided further evidence that the Melbourne detections originated from this radiopharmaceutical production facility. These findings do not have public health implications. This is the first comprehensive study of atmospheric radioxenon measurements and releases in Australia.     

Residual radioactive contamination at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" in the Republic of Sakha (Yakutia)

In this paper, results are reported on the concentrations and activity ratios of 137Cs, 239+240Pu and 238Pu in soils, lichen and bottom sediments collected at the peaceful underground nuclear explosion sites "Craton-3" and "Crystal" (Republic of Sakha (Yakutia), North-East Siberia). At the "Craton-3" site, 239- 240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g in surface soils (0-5 cm) and 239+240Pu concentrations up to 7.4 Bq/g in lichen were observed. The 137Cs concentration in measured soils range from 0.52 to 216 Bq/g for the near-plume and from 1.65 to 21.5 Bq/g for the far-plume. In lichen, 137Cs concentration varied from a global background level up to 251 Bq/g. Radioactive contamination at "Crystal" demonstrates an extremely irregular distribution of 239,240Pu and 137Cs in environmental samples taken at locations within 150 m radius of the site. Further work on compiling detailed maps of radioactive contamination of the territory around "Craton-3" and "Crystal" is discussed.     

A new approach to estimate nuclide ratios from measurements with activities close to background

Measurements of low-level radioactivity often give results of the order of the detection limit. For many applications, interest is not only in estimating activity concentrations of a single radioactive isotope, but focuses on multi-isotope analyses, which often enable inference on the source of the activity detected (e.g. from activity ratios). Obviously, such conclusions become questionable if the measurement merely gives a detection limit for a specific isotope. This is particularly relevant if the presence of an isotope, which shows a low signal only (e.g. due to a short half-life or a small transition probability), is crucial for gaining the information of interest.     

Surface ground contamination and soil vertical distribution of 137Cs around two underground nuclear explosion sites in the Asian Arctic, Russia

Vertical distributions of 137Cs have been determined in vegetation-soil cores obtained from 30 different locations around two underground nuclear explosion sites--"Crystal" (event year - 1974) and "Kraton-3" (event year - 1978) in the Republic of Sakha (Yakutia), Russia. In 2001-2002, background levels of 137Cs surface contamination densities on control forest plots varied from 0.73 to 0.97 kBq m(-2) with an average of 0.84+/-0.10 kBq m(-2) and a median of 0.82 kBq m(-2). 137Cs ground contamination densities at the "Crystal" site ranged from 1.3 to 64 kBq m(-2); the activity gradually decreased with distance from the borehole. For "Kraton-3", residual surface contamination density of radiocaesium varied drastically from 1.7 to 6900 kBq m(-2); maximal 137Cs depositions were found at a "decontaminated" plot. At all forest plots, radiocaesium activity decreased throughout the whole vertical soil profile. Vertical distributions of 137Cs in soil for the majority of the plots sampled (n=18) can be described using a simple exponential function. Despite the fact that more than 20 years have passed since the main fallout events, more than 80% of the total deposited activity was found in the first 5 cm of the vegetation-soil cores from most of the forested landscapes. The low annual temperatures, clay-rich soil type with neutral pH, and presence of thick lichen-moss carpet are the factors which may hinder 137Cs transport down the soil profile.     

228Ra/226Ra/224Ra and 87Sr/86Sr isotope relationships for determining interactions between ground and river water in the upper Rhine valley

Ground and river waters of the upper Rhine valley (Alsace, France) were investigated for chemical composition of the major elements, Sr isotopes and radionuclides from the U and Th series. In particular, the isotope ratios and concentrations of Ra and Sr were used as geochemical tracers to distinguish between different types of water and their interactions. The bulk chemical analyses suggest that the surface waters in the Rhine valley can be described as mixtures between Ca-Na-HCO3-rich ground water and less mineralized slightly acidic river waters which have migrated through crystalline (mainly granitic) basement rocks of the Vosges mountains. Mixing of these waters yields positive correlation between bulk Sr, U, Ca and HCO3, indicating that carbonate-rich sediments are the main source of U and (non-radiogenic) Sr in the Rhine valley aquifers. The combination of the Ra and Sr isotope systems (228Ra/226Ra, 87Sr/86Sr) shows, however, that probably three sources contribute to the surface river waters in the upper Rhine valley, i.e. (i) a highly radiogenic crystalline component, (ii) a ground water source and, (iii) a third component from infiltrating Rhine water along the flow path of the parallel running river Ill in the northerly direction. The Sr and Ra isotope systems were also used to calculate small-scale mixing fractions of tributaries along the flow path of the Ill. Mixing ratios of non-pure end-member waters were determined using three isotope diagrams (i.e. 224Ra/226Ra vs. 228Ra/226Ra) and the results obtained with the Ra isotope system were found to be consistent with the data using Sr isotope relationships (i.e. 87Sr/86Sr vs. 1/Sr).