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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.
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   

3.
Isotopic and elemental compositions of rare gases in various types of gas samples collected in the Japanese Islands were investigated. Excess3He was found in most samples. Many samples showed a regionally uniform high3He/4He ratio of about 7 times the atmospheric ratio. The He concentrations varied from 0.6 to 1800 ppm, and they were low in CO2-rich gases and high in N2-rich gases. Ne isotopic deviations from the atmospheric Ne were detected in most volcanic gases. The deviations and the elemental abundance patterns in volcanic gases can be explained by a mixing between two components, one is mass fractionated rare gases and the other is isotopically atmospheric and is enriched in heavy rare gas elements. Ar was a mixture of mass fractionated Ar, atmospheric Ar and radiogenic Ar, and the contribution of radiogenic40Ar was small in all samples. Except for He, elemental abundance patterns were progressively enriched in the heavier rare gases relative to the atmosphere. Several samples were highly enriched in Kr and Xe relative to the abundance pattern of dissolution equilibrium of atmospheric rare gases in water. The component which is highly enriched in heavy rare gases may be released from sedimentary materials in the crust.  相似文献   

4.
The abundances and isotopic compositions of noble gases in two samples from ultramafic xenoliths in alkali basalt, a young kaersutitic amphibole separated from a peridotite xenolith from Dish Hill, California and an ancient whole-rock lherzolite xenolith from Baja California, are reported and compared with the results of analyses on other mantle samples. In addition to previously recognized excesses of 3He and 129Xe, our results indicate that ambient gases in the mantle show a general enrichment of the lighter-mass nonradiogenic isotopes of Ar, Kr and Xe, and Ar with 40Ar/36Ar = 3 · 102.  相似文献   

5.
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   

6.
We have developed a closed-system combustion technique and utilized it to progressively oxidize a gas-rich, highly carbonaceous acid residue and a fine-grained (<4 μm) matrix sample from the Allende C3V meteorite and analyze the released gases mass spectrometrically. For the residue complete gas mobilization occurs at temperatures below 600°C. The temperature interval over which most of the gases are released coincides with that for combustion of most of the carbon. Release is primarily due to chemical attack rather than thermal activation of the gases. There are somewhat different oxidation thresholds for the heavy gases (Ar, Kr, and Xe) and the light gases (He, Ne), indicating chemically different sites for the two groups. Relative enhancement of isotopically anomalous components near 600°C is as large as in any open-system oxidation method. Differential combustion of the matrix sample reveals three distinct outgassing peaks, the first matching the release from the carbonaceous residue (“combustibles”), the second attributed to sulfides, and the third tentatively assigned to silicates. They comprise about 53%, 7% and 40% of the total heavy gases respectively. While the “sulfides” exhibit a small fission-like component, the Xe in the “silicates” appears isotopically uniform with roughly AVCC composition. The “combustibles” of the matrix contain relatively less excess129Xe than the residue, perhaps indicating that ~10% of the total129Xe in the residue was acquired from “silicates” by redistribution during acid treatment. We cannot rule out the possibility that planetary gases assigned to “sulfides” or “silicates” actually reside in carbonaceous phases somehow sheltered within soluble mineral assemblages, or in acid-soluble carbonaceous phases resistant to oxidation. Integrated releases below and above 600°C during the matrix combustion exhibit virtually identical heavy gas elemental composition, implying similar fractionation during planetary gas entrapment in various materials or in the same material in various environments.  相似文献   

7.
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   

8.
Noble and active gases are released from geological samples during gas extraction for noble gas isotope analyses. The active gases should be removed before inletting to mass spectrometers for the analyses. The normal noble gas preparation systems can clean up most geological samples. However, authigenic minerals from sedimentary rocks in oil/gas fields contain organic matter, which cannot be cleaned up by the normal preparation systems and thus influence the noble gas analyses. We introduce a novel gas purification system(PRC patent No. ZL201320117751.2), which includes several reversible purification pumps with different absorbing and degassing temperatures. It can well clean up water steam, carbon dioxide and organic gases. Mica minerals are often used for ~40Ar/~39 Ar dating. A muscovite sample(2082MS) which could not be cleaned up by the normal preparation system with two SAES NP10~#174; getters, becomes the test sample for a comparative experiment in this study. The experiment is assigned into 4 sections with the organic gas removal system(OGRS) "Closed/Opened" in turn. When the OGRS is closed only with two NP10 getters for purification, the ~40Ar intensities increase in curves with inlet time because of impurities, the ~40Ar/~39 Ar dating results yield age errors about ±2%–±1%(2σ). When the OGRS is opened for purification, in contrast, the ~40 Ar intensities decrease linearly with inlet time. This indicates that the gases have been cleaned up effectively, and the 4~0Ar/~39 Ar results yield ages with errors in ±0.4%. The OGRS is very helpful to obtain high-quality analysis data.  相似文献   

9.
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   

10.
This study presents new major and trace element, mineral, and Sr, Nd, and noble gas isotope geochemical analyses of basalts, gabbro, and clinopyroxenite from the Mariana Arc (Central Islands and Southern Seamount provinces) including the forearc, and the Mariana Trough (Central Graben and Spreading Ridge). Mantle source compositions beneath the Mariana Arc and the Mariana Trough indicate a mantle source that is depleted in high field strength elements relative to MORB (mid‐oceanic ridge basalt). Samples from the Mariana Arc, characterized by high ratios of Ba/Th, U/Th, 84Kr/4He and 132Xe/4He, are explained by addition of fluid from the subducted slab to the mantle wedge. Correlations of noble gas data, as well as large ion lithophile elements, indicate that heavy noble gases (Ar, Kr, and Xe) provide evidence for fluid fluxing into the mantle wedge. On the other hand, major elements and Sr, Nd, He, and Ne isotopic data of basalts from the Mariana Trough are geochemically indistinguishable from MORB. Correlations of 3He/4He and 40Ar/36Ar in the Mariana Trough samples are explained by mixing between MORB and atmosphere. One sample from the Central Graben indicates extreme enrichment in 20Ne/22Ne and 21Ne/22Ne, suggesting incorporation of solar‐type Ne in the magma source. Excess 129Xe is also observed in this sample suggesting primordial noble gases in the mantle source. The Mariana Trough basalts indicate that both fluid and sediment components contributed to the basalts, with slab‐derived fluids dominating beneath the Spreading Ridge, and that sediment melts, characterized by high La/Sm and relatively low U/Th and Zr/Nb, dominate in the source region of basalts from the Central Graben.  相似文献   

11.
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   

12.
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   

13.
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   

14.
Stepwise heating experiments on separated graphite-diamond-kamacite aggregates have revealed a pronounced difference in the release patterns of spallogenic3He and trapped gases. About half the3He is released at T ? 920°C, without being accompanied by significant amounts of primordial gases; the latter, together with the remaining3He, is given off only at T ? 1200°C. Acid treatment of an aliquant dissolved about 2/3 of the total Fe in the sample but did not cause a significant change in the gas concentrations. It is concluded that (a) there is no evidence for a loss of spallogenic3He from the graphite-diamond-kamacite aggregates, (b) one major constituent of the aggregates - graphite - is almost void of trapped gases, (c) kamacite is not a main carrier of the gases. This leaves diamond as the most probable site of the primordial gases.The elemental abundance pattern in the noble gases is essentially as reported previously. In particular, the excellent correlation between relative depletion factors, normalized to the cosmic abundance ratios, and the respective ionisation energies is confirmed. Other important features of the trapped gases are a20Ne/22Ne ratio of 12.3 ± 0.6, intermediate between solar wind and solar flare implanted Ne,36Ar/38Ar = 5.20 ± 0.06 and a measured40Ar/36Ar ratio (before blank correction) of 0.0076.Possible modes of trapping of the noble gases are discussed.  相似文献   

15.
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   

16.
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 2·105–2·10J/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   

17.
Abundances and isotopic compositions of all the stable noble gases have been measured in 19 different depths of the Apollo 15 deep drill core, 7 different depths of the Apollo 16 deep drill core, and in several surface fines and breccias. All samples analyzed from both drill cores contain large concentrations of solar wind implanted gases, which demonstrates that even the deepest layers of both cores have experienced a lunar surface history. For the Apollo 15 core samples, trapped4He concentrations are constant to within a factor of two; elemental ratios show even greater similarities with mean values of4He/22Ne= 683±44,22Ne/36Ar= 0.439±0.057,36Ar/84Kr= 1.60±0.11·103, and84Kr/132Xe= 5.92±0.74. Apollo 16 core samples show distinctly lower4He contents,4He/22Ne(567±74), and22Ne/36Ar(0.229±0.024), but their heavy-element ratios are essentially identical to Apollo 15 core samples. Apollo 16 surface fines also show lower values of4He/22Ne and22Ne/36Ar. This phenomenon is attributed to greater fractionation during gas loss because of the higher plagioclase contents of Apollo 16 fines. Of these four elemental ratios as measured in both cores, only the22Ne/36Ar for the Apollo 15 core shows an apparent depth dependance. No unambiguous evidence was seen in these core materials of appreciable variations in the composition of the solar wind. Calculated concentrations of cosmic ray-produced21Ne,80Kr, and126Xe for the Apollo 15 core showed nearly flat (within a factor of two) depth profiles, but with smaller random concentration variations over depths of a few cm. These data are not consistent with a short-term core accretion model from non-irradiated regolith. The Apollo 15 core data are consistent with a combined accretion plus static time of a few hundred million years, and also indicate variable pre-accretion irradiation of core material. The lack of large variations in solar wind gas contents across core layers is also consistent with appreciable pre-accretion irradiation. Depth profiles of cosmogenic gases in the Apollo 16 core show considerably larger concentrations of cosmogenic gases below ~65 cm depth than above. This pattern may be interpreted either as an accretionary process, or by a more recent deposition of regolith to the upper ~70 cm of the core. Cosmogenic gas concentrations of several Apollo 16 fines and breccias are consistent with ages of North Ray Crater and South Ray Crater of ~50·106 and ~2·106 yr, respectively.  相似文献   

18.
All twenty-three stable rare gas isotopes have been measured in a mantle-derived amphibole, kaersutite. The elemental abundance pattern of the rare gases is similar to the “planetary” rare gas pattern as defined by carbonaceous chondrites. The3He/4He ratio, (4.9 ± 0.6) × 10?5, is suggestive of primordial He degassing from the mantle. Excess21Ne is present. The measured40Ar/36Ar ratio,400 ± 5, may represent a mantle40Ar/36Ar ratio <240 when corrected for radiogenic40Ar. The heavy isotopes of Kr and t0he Xe isotopes are within error of the atmosphere values.  相似文献   

19.
Alpine biotites containing excess40Ar have been analysed by step-heating argon analysis of both neutron irradiated and unirradiated samples. In addition to age spectra the data are discussed in terms of the thermal release of40Ar,39Ar,37Ar and36Ar and also displayed on a correlation plot of36Ar/40Ar vs.39Ar/40Ar which is used to interpret the data and present a model of isotopic evolution during metamorphic cooling. This diagram overcomes misleading complications of isochron plots. The samples exhibit the following argon systematics: (1) flat age spectra for 80–90%39Ar release with anomalously old ages but early gas fractions that approximate the accepted cooling ages; (2) each sample shows decreasing36Ar/40Ar with increasing temperature of heating step with three samples having a negative correlation of36Ar/40Ar vs.39Ar/40Ar and one a positive correlation; (3) there appear to be two36Ar components, one released at high temperatures and correlated with radiogenic40Ar and one released at low temperatures which is not correlated with radiogenic40Ar; and (4) there is no significant effect of neutron irradiation on the release of40Ar and36Ar.Interpretation suggests that these biotites contain a record of the evolution and isotopic composition of ambient argon retained within the metamorphic host rocks during cooling. After incorporation of argon of high40Ar/36Ar another argon component, of atmospheric composition, was retained at lower temperature and argon partial pressures.  相似文献   

20.
Fifteen submarine glasses from the East Pacific Rise (CYAMEX), the Kyushu-Palau Ridge (DSDP Leg 59) and the Nauru Basin (DSDP Leg 61) were analysed for noble gas contents and isotopic ratios. Both the East Pacific Rise and Kyushu-Palau Ridge samples showed Ne excess relative to Ar and a monotonic decrease from Xe to Ar when compared with air noble gas abundance. This characteristic noble gas abundance pattern (type 2, classified by Ozima and Alexander) is interpreted to be due to a two-stage degassing from a noble gas reservoir with originally atmospheric abundance. In the Kyushu-Palau Ridge sample, noble gases are nearly ten times more abundant than in the East Pacific Rise samples. This may be attributed to an oceanic crust contamination in the former mantle source.There is no correlation between the He content and that of the other noble gas in the CYAMEX samples. This suggests that He was derived from a larger region, independent from the other noble gases.Except where radiogenic isotopes are involved, all other noble gas isotopic ratios were indistinguishable from air noble gas isotopic ratios. The3He/4He in the East Pacific Rise shows a remarkably uniform ratio of (1.21±0.07)×10?5, while the40Ar/36Ar ranges from 700 to 5600.  相似文献   

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