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1.
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   

2.
A global monitoring system for atmospheric 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 135I, 133I and 131I. The goal is to distinguish nuclear explosion sources from civilian releases. Simulated nuclear explosion releases along with observational data of radioiodine releases from historic nuclear explosions at the Nevada Test Site are compared to simulated light water reactor releases in order to provide a proof of concept for source discrimination based on radioiodine isotopic activity ratios.  相似文献   

3.
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   

4.
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   

5.
Monitoring of Xe and Kr radionuclides was conducted from August 2006 to 30 July 2008 within the framework of ISTC Project #2133. Cherepovets City in Vologda Province and St. Petersburg were chosen as monitoring locations. Kr–Xe concentrate samples were obtained as a result of processing of several thousand m3 of atmospheric air. New results of 85Kr monitoring show, that for last 15 years, the 85Kr volumetric activity in the atmospheric air of the northwest region of Russia has increased approximately 50% and has achieved a level of 1.5 Bq/m3. This value correlates well with similar data for Western Europe and Japan. The xenon fraction (80–160 cm3 under STP) is adsorbed on charcoal in the ampoule, which is measured in the well of HPGe gamma detector. Minimum detectable concentration (MDC) of 133Xe for this technique is 0.008 mBq/m3, and it is the most sensitive method used today. The 133Xe concentration in the atmospheric air of Cherepovets City varied in the monitoring period ranging from 0.09 to 2.5 mBq/m3. During the period of March 2007–30 July 2008, 133Xe activity concentration in the atmospheric air of St. Petersburg changed from background values (0.2–0.3 mBq/m3) to 185 mBq/m3 and for approximately 20% of the samples 135Xe was also measured with the 135Xe/133Xe activity ratio varied within the range of 0.03–3.5.  相似文献   

6.
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   

7.
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   

8.
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   

9.
Cores and coats of five coated diamonds, one from Botswana and four from Zaire, were separately analyzed for their noble gases. Noble gases in the diamonds are essentially of a trapped origin, including radio- and nucleogenic components such as4He, 40Ar, 21Neexcess and excesses in Xe isotopes (129, 131–136). The fairly precise elemental and isotopic abundances allow us to infer the noble gas state in the ancient mantle. 20Ne/22Ne ratios are fairly constant (11.8 ± 0.4), and very close to that of SEP (solar energetic particle)-Ne, but distinctly different from the atmospheric ratio. 21Ne/22Ne ratios range from 0.028 to 0.06, which is attributed to nucleogenic 21Ne from 18O(α, n)21Ne and 24Mg(n, α)21Ne reactions. The difference in 20Ne/22Ne between atmosphere and mantle can be attributed to the hydrodynamic escape of hydrogen from the primitive atmosphere during the very early stage in the Earth's history. 38Ar/36Ar and Kr isotopic ratios are identical to the atmospheric values within 1%. After correction for 238U- or 244Pu-fission Xe, the 131–136Xe abundance ratios are indistinguishable from atmospheric ratios. Lighter Xe isotopes (124–128Xe) are also likely to be atmospheric, but a final conclusion must wait until better data are obtained.In a 136Xe/130Xe−129Xe/130Xe diagram, diamond data lie on the same line as defined for MORB. The observed identical correlation for both diamonds and MORB's appears to suggest that the progenitor of the excess131–136Xe is 244Pu, but not238U, though the direct Xe isotopic measurements was not precies enough to decide unanimously the progenitor.  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.
Detonation gases released by an underground nuclear test include trace amounts of 133Xe and 37Ar. In the context of the Comprehensive Nuclear Test Ban Treaty, On Site Inspection Protocol, such gases released from or sampled at the soil surface could be used to indicate the occurrence of an explosion in violation of the treaty. To better estimate the levels of detectability from an underground nuclear test (UNE), we developed mathematical models to evaluate the processes of 133Xe and 37Ar transport in fractured rock. Two models are developed respectively for representing thermal and isothermal transport. When the thermal process becomes minor under the condition of low temperature and low liquid saturation, the subsurface system is described using an isothermal and single-gas-phase transport model and barometric pumping becomes the major driving force to deliver 133Xe and 37Ar to the ground surface. A thermal test is simulated using a nonisothermal and two-phase transport model. In the model, steam production and bubble expansion are the major processes driving noble gas components to ground surface. After the temperature in the chimney drops below boiling, barometric pumping takes over the role as the major transport process.  相似文献   

12.
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   

13.
The abundance and isotopic composition of noble gases were determined in samples of CO2 well gas from Harding County, New Mexico. Our results confirm the presence of radiogenic129Xe and fissiogenic131–136Xe. Relative to noble gases in air, the CO2 gas is selectively depleted in the lighter weight, nonradiogenic noble gases, except at neon. It is suggested that loss of atmospheric neon into space could account for an apparent excess of neon in juvenile gases.  相似文献   

14.
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   

15.
Monitoring of radioactive noble gases, in particular xenon isotopes, is a crucial element of the verification of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). The capability of the noble gas network, which is currently under construction, to detect signals from a nuclear explosion critically depends on the background created by other sources. Therefore, the global distribution of these isotopes based on emissions and transport patterns needs to be understood. A significant xenon background exists in the reactor regions of North America, Europe and Asia. An emission inventory of the four relevant xenon isotopes has recently been created, which specifies source terms for each power plant. As the major emitters of xenon isotopes worldwide, a few medical radioisotope production facilities have been recently identified, in particular the facilities in Chalk River (Canada), Fleurus (Belgium), Pelindaba (South Africa) and Petten (Netherlands). Emissions from these sites are expected to exceed those of the other sources by orders of magnitude. In this study, emphasis is put on 133Xe, which is the most prevalent xenon isotope. First, based on the emissions known, the resulting 133Xe concentration levels at all noble gas stations of the final CTBT verification network were calculated and found to be consistent with observations. Second, it turned out that emissions from the radioisotope facilities can explain a number of observed peaks, meaning that atmospheric transport modelling is an important tool for the categorization of measurements. Third, it became evident that Nuclear Power Plant emissions are more difficult to treat in the models, since their temporal variation is high and not generally reported. Fourth, there are indications that the assumed annual emissions may be underestimated by factors of two to ten, while the general emission patterns seem to be well understood. Finally, it became evident that 133Xe sources mainly influence the sensitivity of the monitoring system in the mid-latitudes, where the network coverage is particularly good.  相似文献   

16.
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   

17.
Rare gas isotopes in a phlogopite nodule and a phlogopite-bearing peridotite nodule in South African kimberlites were studied to examine the state of rare gases in the deep interior of the kimberlite region.Within the experimental error of 1 ～ 2%, rare gas isotopic compositions are atmospheric except for radiogenic4He and40Ar. No excess129Xe was observed.In phlogopite, Ne is more depleted, whereas the heavier rare gases are more enriched than the atmospheric rare gases relative to36Ar.Together with other data these results suggest that the state of rare gases in the upper mantle of the South African kimberlite region might have been changed from the typical primitive mantle by a process such as mixing of crustal materials.  相似文献   

18.
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   

19.
A new method to date uranium-bearing minerals exclusively by means of a mass spectrometric determination of Xe and/or Kr isotopic ratios has been developed and experimentally tested. It is based on the compositional differences between Xe produced by spontaneous fission of238U in nature and Xe from235U fission induced by thermal neutrons in a nuclear reactor. Xe is extracted in 5–10 release fractions at successively higher temperatures. This relates the radiogenic Xe contained in various structural elements of different retention characteristics to the respective U concentrations and allows to account for natural Xe losses, which are quite common. A monazite monitor mineral of known age is included in each irradiation and its Xe isotopes are measured in the same way.The samples analyzed include uranium oxides, REE phosphates, tantalum niobates, zircon and others.The results and comparisons with reported ages obtained by other means demonstrate the applicability of the new dating method for minerals with U contents up to a few percent. In age spectra the low-temperature release fractions of some samples indicate radiogenic Xe losses, while at high temperatures age plateaux can be obtained.  相似文献   

20.
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   

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