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1.
Activity concentration data from ambient radioxenon measurements in ground level air, which were carried out in Europe in the framework of the International Noble Gas Experiment (INGE) in support of the development and build-up of a radioxenon monitoring network for the Comprehensive Nuclear-Test-Ban Treaty verification regime are presented and discussed. Six measurement stations provided data from 5 years of measurements performed between 2003 and 2008: Longyearbyen (Spitsbergen, Norway), Stockholm (Sweden), Dubna (Russian Federation), Schauinsland Mountain (Germany), Bruyères-le-Châtel and Marseille (both France). The noble gas systems used within the INGE are designed to continuously measure low concentrations of the four radioxenon isotopes which are most relevant for detection of nuclear explosions: 131mXe, 133mXe, 133Xe and 135Xe with a time resolution less than or equal to 24 h and a minimum detectable concentration of 133Xe less than 1 mBq/m3. This European cluster of six stations is particularly interesting because it is highly influenced by a high density of nuclear power reactors and some radiopharmaceutical production facilities. The activity concentrations at the European INGE stations are studied to characterise the influence of civilian releases, to be able to distinguish them from possible nuclear explosions. It was found that the mean activity concentration of the most frequently detected isotope, 133Xe, was 5–20 mBq/m3 within Central Europe where most nuclear installations are situated (Bruyères-le-Châtel and Schauinsland), 1.4–2.4 mBq/m3 just outside that region (Stockholm, Dubna and Marseille) and 0.2 mBq/m3 in the remote polar station of Spitsbergen. No seasonal trends could be observed from the data. Two interesting events have been examined and their source regions have been identified using atmospheric backtracking methods that deploy Lagrangian particle dispersion modelling and inversion techniques. The results are consistent with known releases of a radiopharmaceutical facility.  相似文献   

2.
Atmospheric measurement of radioactive xenon isotopes (radioxenon) plays a key role in remote monitoring of nuclear explosions, since it has a high capability to capture radioactive debris for a wide range of explosion scenarios. It is therefore a powerful tool in providing evidence for nuclear testing, and is one of the key components of the verification regime of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The reliability of this method is largely based on a well-developed measurement technology. In the 1990s, with the prospect of the build-up of a monitoring network for the CTBT, new development of radioxenon equipment started. This article summarizes the physical and technical principles upon which the radioxenon technology is based and the advances the technology has undergone during the last 10 years. In contrast to previously used equipment, which was manually operated, the new generation of radioxenon monitoring equipment is designed for automated and continuous operation in remote field locations. Also the analytical capabilities of the equipment were strongly enhanced. Minimum detectable concentrations of the recently developed systems are well below 1 mBq/m3 for the key nuclide 133Xe for sampling periods between 8 and 24 h. All the systems described here are also able to separately measure with low detection limits the radioxenon isotopes 131mXe, 133mXe and 135Xe, which are also relevant for the detection of nuclear tests. The equipment has been extensively tested during recent years by operation in a laboratory environment and in field locations, by performing comparison measurements with laboratory type equipment and by parallel operation. These tests demonstrate that the equipment has reached a sufficiently high technical standard for deployment in the global CTBT verification regime.  相似文献   

3.
Both radioxenon and radioiodine are possible indicators for a nuclear explosion. Therefore, they will be, together with other relevant radionuclides, globally monitored by the International Monitoring System in order to verify compliance with the Comprehensive Nuclear-Test-Ban Treaty once the treaty has entered into force. This paper studies the temporal development of radioxenon and radioiodine activities with two different assumptions on fractionation during the release from an underground test. In the first case, only the noble gases are released, in the second case, radioiodine is released as well while the precursors remain underground. For the second case, the simulated curves of activity ratios are compared to prompt and delayed atmospheric radioactivity releases from underground nuclear tests at Nevada as a function of the time of atmospheric air sampling for concentration measurements of 135I, 133I and 131I. In addition, the effect of both fractionation cases on the isotopic activity ratios is shown in the four-isotope-plot (with 135Xe, 133mXe, 133Xe and 131mXe) that can be utilized for distinguishing nuclear explosion sources from civilian releases.  相似文献   

4.
A global monitoring system for atmospheric xenon radioactivity is being established as part of the International Monitoring System that will verify compliance with the Comprehensive Nuclear-Test-Ban Treaty (CTBT) once the treaty has entered into force. This paper studies isotopic activity ratios to support the interpretation of observed atmospheric concentrations of 135Xe, 133mXe, 133Xe and 131mXe. The goal is to distinguish nuclear explosion sources from civilian releases. Simulations of nuclear explosions and reactors, empirical data for both test and reactor releases as well as observations by measurement stations of the International Noble Gas Experiment (INGE) are used to provide a proof of concept for the isotopic ratio based method for source discrimination.  相似文献   

5.
The value of the 133Xe/133mXe isometric activity ratio for the stationary regime of reactor work is about 35, and that for an instant fission (explosion) is about 11, which allowed estimation of the nuclear component of the instant (explosion) energy release during the NPP accident. Atmospheric xenon samples were taken at the trajectory of accident product transfers (in the Cherepovetz area); these samples were measured by a gamma spectrometer, and the 133Xe/133mXe ratio was determined as an average value of 22.4. For estimations a mathematic model was elaborated considering both the value of instant released energy and the schedule of reactor power change before the accident, as well as different fractionation conditions on the isobaric chain. Comparison of estimated results with the experimental data showed the value of the instant specific energy release in the Chernobyl NPP accident to be 2·105–2·106 J/Wt or 6·1014–6·1015 J (100–1,000 kt). This result is matched up to a total reactor power of 3,200 MWt. However this estimate is not comparable with the actual explosion scale estimated as 10t TNT. This suggests a local character of the instant nuclear energy release and makes it possible to estimate the mass of fuel involved in this explosion process to be from 0.01 to 0.1% of total quantity.  相似文献   

6.
Atmospheric noble gases (e.g., 22Ne, 36Ar, 84Kr, 130Xe) in crustal fluids are only sensitive to subsurface physical processes. In particular, depletion of atmospheric noble gases in groundwater due to boiling and steam separation is indicative of the occurrence of a thermal event and can thus be used to trace the thermal history of stable tectonic regions. We present noble gas concentrations of 38 deep brines (~ 0.5–3.6 km) from the Michigan Basin. The atmospheric noble gas component shows a strong depletion pattern with respect to air saturated water. Depletion of lighter gases (22Ne and 36Ar) is stronger compared to the heavier ones (84Kr and 130Xe). To understand the mechanisms responsible for this overall atmospheric noble gas depletion, phase interaction models were tested. We show that this atmospheric noble gas depletion pattern is best explained by a model involving subsurface boiling and steam separation, and thus, consistent with the occurrence of a past thermal event of mantle origin as previously indicated by both high 4He/heat flux ratios and the presence of primordial mantle He and Ne signatures in the basin. Such a conceptual model is also consistent with the presence of past elevated temperatures in the Michigan Basin (e.g., ~ 80–260 °C) at shallow depths as suggested by previous thermal studies in the basin. We suggest that recent reactivation of the ancient mid-continent rift system underneath the Michigan Basin is likely responsible for the release of both heat and mantle noble gases into the basin via deep-seated faults and fracture zones. Relative enrichment of atmospheric Kr and Xe with respect to Ar is also observed, and is interpreted as reflecting the addition of sedimentary Kr and Xe from associated hydrocarbons, following the hydrothermal event. This study pioneers the use of atmospheric noble gases in subsurface fluids to trace the thermal history of stable tectonic regions.  相似文献   

7.
During on-site inspections to verify the comprehensive nuclear-test-ban treaty (CTBT), soil gas samples may be taken and analysed for their content of the xenon isotopes 131mXe, 133Xe, 133mXe and 135Xe in order to identify a suspected underground nuclear test. These samples might contain natural radioxenon which is present as a trace gas in the ground. This work analyses the different production mechanisms of natural lithospheric radioxenon to assess theoretically the background concentration under different sampling conditions. The results imply that the equilibrium concentrations of the examined xenon isotopes can be measured in certain rock types using actual CTBTO on-site inspection equipment. Radioxenon production is dominated by spontaneous fission of 238U, resulting in a reactor-like xenon isotopic signature rather than an explosion-like signature.  相似文献   

8.
The announced October 2006 nuclear test explosion in the Democratic People’s Republic of Korea (DPRK) has been the first real test regarding the technical capabilities of the verification system built up by the Vienna-based Provisional Technical Secretariat (PTS) of the Comprehensive Nuclear-Test-Ban Treaty Organization (CTBTO) to detect and locate a nuclear test event. This paper enhances the resolution of the DPRK events’ xenon source reconstruction published by Saey et al. (2007, “A long distance measurement of radioxenon in Yellowknife, Canada, in late October 2006”, GRL, Vol. 34, L20802) that was based solely on radio-xenon measurements taken at the remote radionuclide station in Yellowknife, Canada by involving additional measurements taken by a mobile noble gas system deployed quite close to the event location in the Republic of Korea (ROK). Moreover the horizontal resolution of the forward and backward atmospheric transport modelling methods applied for the source scenario reconstruction has been enhanced appropriately to reflect the considerably shorter source-receptor distances examined in comparison to the previously published source reconstruction. It is shown that the 133Xe measurements in Yellowknife could register 133Xe traces from the nuclear explosion during the first 3 days after the event, while the mobile measurements were rather sensitive to releases during days 2–4 after the explosion. According to the analysis, the most likely source scenario would consist of an initial (possibly up to 21 h delayed) venting of 1 × 10?15 Bq 133Xe during the first 24 h, followed by a two orders of magnitude weaker seepage during the following 3 days. Both measurements corroborate the scenario of a rather rapid venting and soil diffusion of the 133Xe yielded during the explosion. While the Swedish mobile measurements were crucial to enhancement of the reconstruction of the source scenario, given the installation status of the IMS xenon network at the time of the event, a sensitivity analysis revealed that the fully developed network would have been able to detect 133Xe traces from the Korean explosion at a number of stations and allowed for an even better constraint on the release function. The station Ussuriysk, Russia, being in operation in 2006, would have registered 133Xe within 1 day and with a three orders of magnitudes stronger signal compared to the detection at Yellowknife.  相似文献   

9.
Few studies in the Middle East region estimated the spatial distribution of air pollutants for exposure studies. This paper presents a geostatistical approach to assess background NO2 spatial distribution and the associated exposed population in a Mediterranean city with a complex topography, Beirut. Such modeling gave an accurate mapping of the 2010 yearly background average value of NO2: it varies between 35 and 67 μg m?3 with a mean of 53 μg m?3. The mean SD of the estimated error was about 3 μg m?3. The results showed that the spatial distribution of NO2 follows a nested structuring, with a major structure related to topoclimatic characteristics (interaction topography/atmospheric flow at large scale) and a minor one linked to micro-environment and micro-climatic characteristics (interactions urban morphology/atmospheric flows at fine scale). The probability for the city’s inhabitants to be exposed to NO2 levels exceeding 40 μg m?3 threshold limit set by the World Health Organization (WHO) showed that Beirut city has a real sanitary risk to the NO2 pollution. 93 % of the population (around 358,459 people) is 100 % sure to be exposed to a yearly average exceeding 40 μg m?3. This knowledge will be certainly useful for developing a tool for decision support in order to implement policies of reducing air pollution in Beirut, which is, given the results, very urgent.  相似文献   

10.
36Ar, 84Kr, and 132Xe abundances along with Kr and Xe isotopic compositions are reported for two African shales and samples of chert from the Gunflint Formation in Canada. It is observed that these data and similar abundance data from other terrestrial materials show correlations between 36Ar-84Kr and between 84Kr-132Xe. The elemental ratios defined by all the above data differ significantly from and show greater variations than those measured in carbonaceous chondrites, a well-investigated class of extraterrestrial material. Physical absorption and equilibrium solubility acting on the atmosphere are investigated as explanations for the observations. The Kr and Xe isotopic spectra are also consistent with a mass-dependent incorporation process acting on a reservoir of atmospheric composition.  相似文献   

11.
In this paper we report Ne, Ar, Kr and Xe analyses of josephinite, Josephine Peridotite, and serpentinized Josephine Peridotite. In all three samples the elemental abundance patterns resemble patterns associated with surface waters, the Ne data do not exhibit the large21Ne enrichments observed earlier, and the Kr and Xe compositions are indistinguishable from atmospheric composition at all isotopes, including129Xe. Our data thus offer no significant evidence for isotopic anomalies in the noble gases. We also argue that the previous claims for primordial atmospheric-like Ar, anomalous Kr and Xe, excess129Xe, and 4.6 × 109-year age are all questionable interpretations which cannot be defended against more prosaic alternatives. This leaves excess21Ne as the only noble gas argument for exotic origin; we suggest that this might be an experimental artifact. Until the21Ne question can be settled by more definitive experimentation, we feel that noble gas data cannot be used to support arguments that the origin of josephinite is more exotic than crustal serpentinization.  相似文献   

12.
Kr and Xe were measured by a stepwise heating technique in three samples of a drill core in the “Minnesota” fragment of the Estherville mesosiderite. The cosmogenic78Kr/83Kr decreased from the “top” sample to the “bottom” sample(“top” = 0.163 ± 0.005, “bottom” = 0.151 ± 0.005) while the cosmogenic131Xe/126Xe ratio increased(“top” = 5.58 ± 0.35, “bottom” = 6.92 ± 0.17). Cosmic-ray track studies have shown that the “top” sample was indeed closer to the preatmospheric surface than the “bottom” sample by ～ 10 cm. This is the first direct evidence, in a sample of known geometry, that the cosmogenic131Xe/126Xe ratio increases as a function of depth, and as such, confirms the hypothesis that the lunar131Xe anomaly is a bona fide depth effect due to resonance neutron capture in130Ba.  相似文献   

13.
Relative yields of Kr and Xe isotopes from the spontaneous fission of 248Cm and 250Cf have been determined mass spectrometrically. The yields are as follows: 83Kr/84Kr/85Kr/86Kr = 0.223/0.458/0.596/ ≡ 1.00 and 0.306/0.582/0.793/ ≡ 1.00;131Xe/132Xe/134Xe/136Xe = 0.486/0.819/1.075/ ≡ 1.00 and 0.343/0.506/0.851/ ≡ 1.00 from 248Cm and 250Cf, respectively. The Xe yields from 248Cm agree with an earlier determination by Leich et al. [24]. Neither of these yield patterns matches that of “fissiogenic” Kr and Xe in carbonaceous chondrites and hence 248Cm and 250Cf are ruled out as progenitors of the meteoritic Kr and Xe. In general, none of the spontaneously fissioning nuclides of actinide elements can be identified as a possible progenitor. Even the mixtures of actinides, including a combination of 248Cm and 250Cm, are unsuitable. The origin of “anomalous” Kr and Xe in carbonaceous chondrites must then be traced either to the spontaneous fission of a superheavy element or to peculiarities in specific nucleosynthetic reactions.  相似文献   

14.
Radon can be used as a naturally occurring tracer for environmental processes. By means of grab-sampling or continuous monitoring of radon concentration, it is possible to assess several types of dynamic phenomena in air and water. We present a review of the use of radon and its progeny at the University of Cantabria. Radon can be an atmospheric dynamics indicator related with air mass interchange near land-sea discontinuities as well as for the study of vertical variations of air parameters (average values of different types of stability: 131–580 Bq m?3). Concerning indoor gas, we present some results obtained at Altamira Cave (Spain): from 222 to 6549 Bq m?3 (Hall) and from 999 to 6697 Bq m?3 (Paintings Room). Finally, variations of radon concentration in soil (0.3 to 9.1 kBq m?3) and underground water (values up to 500 Bq l?1) provide relevant information about different geophysical phenomena.  相似文献   

15.
Noble gas elemental and isotopic abundances were measured in seven deep-sea water samples from five different sampling sites in the Nankai Trough, the Japan Trench and the Kuril Trench. The samples were obtained by the manned submersible “Nautile”. Most of the sampling sites are associated with clam colonies and/or fluid venting. Excesses both in3He/4He ratio and He concentration are observed in a seawater sample collected a few kilometers off the clam colonies which were found at a depth of 3830 m at the mouth of the Tenryu Canyon. Concentrations of noble gases (Ne, Ar, Kr and Xe) in this sample show progressive depletion from Ne to Xe relative to those in 1°C air-saturated seawater, which can be attributed to mixing of hot water ( 15°C) with cold ambient water ( 1°C). Isotopic compositions of Ne, Ar, Kr and Xe in this sample are atmospheric. These observations may reflect venting of hot pore water around the Tenryu Canyon. All the other samples show a significant excess in concentration of all noble gases relative to 1°C air-saturated seawater and the isotopic compositions are atmospheric. This excess of noble gas concentrations may appear to be air contamination in the samples. However, results of hydrocarbon analyses of the Kaiko samples imply that such large amount of air contamination is improbable. Decomposition of gas hydrate in deep-sea sediments is a more likely explanation for the observed excess of noble gas concentration.  相似文献   

16.
The present part of the publication (Part II) deals with long range dispersion of radionuclides emitted into the atmosphere during the Fukushima Dai-ichi accident that occurred after the March 11, 2011 tsunami. The first part (Part I) is dedicated to the accident features relying on radionuclide detections performed by monitoring stations of the Comprehensive Nuclear Test Ban Treaty Organization network. In this study, the emissions of the three fission products Cs-137, I-131 and Xe-133 are investigated. Regarding Xe-133, the total release is estimated to be of the order of 6 × 1018 Bq emitted during the explosions of units 1, 2 and 3. The total source term estimated gives a fraction of core inventory of about 8 × 1018 Bq at the time of reactors shutdown. This result suggests that at least 80 % of the core inventory has been released into the atmosphere and indicates a broad meltdown of reactor cores. Total atmospheric releases of Cs-137 and I-131 aerosols are estimated to be 1016 and 1017 Bq, respectively. By neglecting gas/particulate conversion phenomena, the total release of I-131 (gas + aerosol) could be estimated to be 4 × 1017 Bq. Atmospheric transport simulations suggest that the main air emissions have occurred during the events of March 14, 2011 (UTC) and that no major release occurred after March 23. The radioactivity emitted into the atmosphere could represent 10 % of the Chernobyl accident releases for I-131 and Cs-137.  相似文献   

17.
The concentrations and isotopic compositions of argon, krypton and xenon have been determined in a grain size suite of zircons separated from pyroxene syenite of the Botnavatn Igneous Complex, southwestern Norway. The UPb systematics of these zircons has been studied previously.Kr and Xe are mixtures of fissiogenic gas from the spontaneous fission of238U and a component with atmospheric isotopic composition. From correlation diagrams the fissiogenic component is determined to be:83Kr :84Kr :86Kr = (4.6 ± 1.3) : (11.0 ± 2.0) : 100 and129Xe :131Xe :132Xe :134Xe :136Xe = (0.6 ± 0.3) : (8.8 ± 0.2) : (56.8 ± 0.3) : (82.8 ± 0.4) : 100. The fissiogenic136Xe/86Kr is 6.0 ± 0.4.The Ar isotopic composition shows radiogenic40Ar and a small excess of38Ar. The excess38Ar of about 1 × 10−11 cm3 STP/g can be explained by reactions of α-particles with chlorine. Asymmetric fission of238U which has been postulated to cause argon isotope anomalies in U-rich minerals is unnecessary to explain the observed38Ar concentrations.UXe ages are (1.19 ± 0.07) Ga, in agreement with UPb ages. However, if the recoil loss of fissiogenic Xe is considered the UXe ages of these zircons are about 1.53 Ga, which is comparable with the KAr ages and some RbSr ages observed in basement rocks in this region. The uncertainty of the product of fission yield times spontaneous fission decay constant of238U prevents to decide which age is the true crystallization age.  相似文献   

18.
Part I of this publication deals with the analysis of fission product releases consecutive to the Fukushima Dai-ichi accident. Reactor core damages are assessed relying on radionuclide detections performed by the CTBTO radionuclide network, especially at the particulate station located at Takasaki, 210 km away from the nuclear power plant. On the basis of a comparison between the reactor core inventory at the time of reactor shutdowns and the fission product activities measured in air at Takasaki, especially 95Nb and 103Ru, it was possible to show that the reactor cores were exposed to high temperature for a prolonged time. This diagnosis was confirmed by the presence of 113Sn in air at Takasaki. The 133Xe assessed release at the time of reactor shutdown (8 × 1018 Bq) turned out to be in the order of 80 % of the amount deduced from the reactor core inventories. This strongly suggests a broad meltdown of reactor cores.  相似文献   

19.
Nitrogen and noble gases were measured in samples of a glass inclusion and the surrounding basaltic matrix from the antarctic shergottite EETA 79001. A nitrogen component trapped in the glass, but not present in the matrix, has a δ15N value at least as high as +190‰. Ratios of40Ar/14N and15N/14N in the glass are consistent with dilution of a martian atmospheric component (δ15N = 620 ± 160‰,40Ar/14N= 0.33 ± 0.03) by either terrestrial atmosphere adsorbed on the samples or by indigenous nitrogen from the minerals of the rock. Trapped noble gases in the glass reproduce, within error, the elemental and isotopic compositions measured in Mars' atmosphere by Viking, and are in general agreement with previous measurements except for much lower abundances of neutron-generated krypton and xenon isotopes. The most reasonable explanation at the present time for the noble gas pattern and the isotopically heavy nitrogen is that a sample of martian atmosphere has been trapped in the EETA 79001 glass, and that this meteorite, and thus the shergottites and probably the nakhlites and chassignites as well, originated on Mars.Nitrogen in the non-glassy matrix of EETA 79001 amounts to less than 0.5 ppm and has a spallation-corrected δ15N value in the range 0 to ?20‰; it may reflect indigenous nitrogen in the basalt or a mixture of indigenous and adsorbed terrestrial nitrogen. Spallogenic noble gases yield single-stage exposure ages between 400,000 and 900,000 years, depending on irradiation geometry. Trapped argon may have an unusually low36Ar/38Ar ratio. Trapped krypton, except for a small excess at80Kr, is smoothly mass-fractionated with respect to either terrestrial or chondritic Kr. The trapped xenon composition is consistent with addition of neutron-capture, radiogenic and fissiogenic isotopes to a base composition resembling terrestrial atmospheric Xe. The elemental84Kr/132Xe ratio of 25 is close to the terrestrial value and very different from the chondritic ratio.  相似文献   

20.
Two adjacent bays in a large oligotrophic lake (Georgian Bay, Lake Huron) were compared to determine how the inputs from relatively pristine, but moderately humic, tributaries may influence phytoplankton, nutrients and system metabolism. Dissolved organic carbon (DOC) concentrations decreased from 4 to 5 gC m?3 at inner sites to 2 gC m?3 or less at outer sites. The concentration gradient from inner to outer was greater in the bay with a major tributary, and optical properties (intensity and slope of light absorption spectrum) showed there was a loss of material with allochthonous characteristics along the gradient. Chlorophyll a (Chl a) and total phosphorus (TP) were also higher at inner (2–4 mg Chl a m?3 and 8–12 mgP m?3, respectively) than outer sites (≤1 mg Chl a m?3 and 4–5 mgP m?3). Chl a and TP, as well as particulate nutrient ratios (C:P, C:N, N:P), indicated significant eutrophication at inner sites, especially in the bay with the tributary, and there was a strong positive Chl a-phosphorus relationship. The stable oxygen isotope ratio (18O:16O) of dissolved oxygen indicated greater influence of biological oxygen fluxes at inner sites (where ratios were 2–3 ppt below atmospheric equilibrium) than at outer sites (where ratios were within 0.5 ppt of equilibrium). Community photosynthesis:respiration ratios inferred from 18O:16O varied positively with Chl a and inorganic nutrients, but negatively with DOC. Altered loading of allochthonous organic matter can be expected under changing climate and development scenarios and will have significant influence on optical properties and system metabolism through changes in DOC in this coastal system. The effects will nonetheless be strongly modulated by any accompanying change in inorganic nutrients.  相似文献   

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