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1.
We performed U–Th radioactive disequilibrium analyses of carbonate nodules and sediment samples recovered from methane seep sites off Joetsu, of the eastern margin of Japan Sea, to decipher the active period of the methane seep. The carbonates contain 230Th, part of which is located in detritus such as silicate and organics, at the time of precipitation. The initial 230Th renders accurate dating with U–Th radioactive disequilibrium method difficult. We assessed the feasibility of correction using radioactive disequilibrium data of ambient sediment to overcome this difficulty. A (230Th/232Th)–(234U/232Th) isochron drawn by three chips divided from a carbonate nodule (PC05-04-50) passed through data points of local sediments. We conclude that the problem of initial 230Th can be resolved by measurements of local sediments. Results show that carbonate nodules include local sediment as impurities. Furthermore, the results of trace element analyses such as Rb, Zr, Nb, REE, Pb, and Th also support the idea.In all, 18 carbonate samples were dated with correction of initial 230Th using the mean value of local sediment in this study. The U–Th correction ages show 12–35ka with an isochron age of 26 ± 3ka. Results indicate that during the time interval of U–Th ages, from 12ka to 35ka, environmental conditions must have been favorable for enhanced methane flux through sediment. The extensive methane flow period at 20ka accords with the lowest-stand sea level during the last glacial age. Results of this study also suggest that U–Th ages of carbonate are useful as a reliable chronometer with regard to methane seep activation. In order to acquire U–Th ages of carbonate at methane seep sites, however, it is important to evaluate the amount of initial 230Th accurately using the value of sediment.  相似文献   

2.
We have developed techniques to measure the230Th abundance in corals by isotope dilution mass spectrometry. This, coupled with our previous development of mass spectrometric techniques for234U and232Th measurement, has allowed us to reduce significantly the analytical errors in238U234U230Th dating and greatly reduce the sample size. We show that 6 × 108 atoms of230Th can be measured to ±30‰ (2σ) and 2 × 1010 atoms of230Th to ±2‰. The time over which useful age data on corals can be obtained ranges from a few years to 500 ky. The uncertainty in age, based on analytical errors, is ±5 y (2σ) for a 180 year old coral (3 g), ±44 y at 8294 years and ±1.1 ky at 123.1 ky (250 mg of coral). We also report232Th concentrations in corals (0.083–1.57 pmol/g) that are more than two orders of magnitude lower than previous values. Ages with high analytical precision were determined for several corals that grew during high sea level stands 120 ky ago. These ages lie specifically within or slightly postdate the Milankovitch insolation high at 128 ky and support the idea that the dominant cause of Pleistocene climate change is Milankovitch forcing.  相似文献   

3.
High spatial resolution U–Pb dates of zircons from two consanguineous ignimbrites of contrasting composition, the high-silica rhyolitic Toconao and the overlying dacitic Atana ignimbrites, erupted from La Pacana caldera, north Chile, are presented in this study. Zircons from Atana and Toconao pumice clasts yield apparent 238U/206Pb ages of 4.11±0.20 Ma and 4.65±0.13 Ma (2σ), respectively. These data combined with previously published geochemical and stratigraphic data, reveal that the two ignimbrites were erupted from a stratified magma chamber. The Atana zircon U–Pb ages closely agree with the eruption age of Atana previously determined by K–Ar dating (4.0±0.1 Ma) and do not support long (>1 Ma) residence times. Xenocrystic zircons were found only in the Toconao bulk ignimbrite, which were probably entrained during eruption and transport. Apparent 238U/206Pb zircon ages of 13 Ma in these xenocrysts provide the first evidence that the onset of felsic magmatism within the Altiplano–Puna ignimbrite province occurred approximately 3 Myr earlier than previously documented.  相似文献   

4.
Fresh basaltic glasses have been analyzed for U&z.sbnd;Th disequilibrium systematics as part of an extensive study on the East Pacific Rise (EPR) at 12°45′N. These samples are well described in terms of major and trace elements as well as in Nd, Pb and Sr isotopes. Our results show significant heterogeneities in the mantle source at a small scale, and show heterogeneities at larger scales also when compared to other EPR data.U and Th concentration and isotopic data rule out fractional crystallization as a main process and support a mixing model in agreement with the marble cake model developed by Alle`gre and Turcotte and constrained by trace elements and Nd, Sr and Pb isotopes on the same samples by Prinzhofer et al.Based on the high ( 230Th/232Th ) isotopic ratios on recent tholeiites especially the Th/U values inferred for their sources clearly show that the upper mantle Th/U has decreased with time.  相似文献   

5.
The precise knowledge of the initial 26Al/27Al ratio [(26Al/27Al)0] is crucial if we are to use the very first solid objects formed in our Solar System, calcium–aluminum-rich inclusions (CAIs) as the “time zero” age-anchor and guide future work with other short-lived radio-chronometers in the early Solar System, as well as determining the inventory of heat budgets from radioactivities for early planetary differentiation. New high-precision multi-collector inductively-coupled plasma mass spectrometry (MC-ICP-MS) measurements of 27Al/24Mg ratios and Mg-isotopic compositions of nine whole-rock CAIs (six mineralogically characterized fragments and three micro-drilled inclusions) from the CV carbonaceous chondrite, Allende yield a well-defined 26Al–26Mg fossil isochron with an (26Al/27Al)0 of (5.23 ± 0.13) × 10− 5. Internal mineral isochrons obtained for three of these CAIs (A44A, AJEF, and A43) are consistent with the whole-rock CAI isochron. The mineral isochron of AJEF with (26Al/27Al)0 = (4.96 ± 0.25) × 10− 5, anchored to our precisely determined absolute 207Pb–206Pb age of 4567.60 ± 0.36 Ma for the same mineral separates, reinstate the “canonical” (26Al/27Al)0 of 5 × 10− 5 for the early Solar System. The uncertainty in (26Al/27Al)0 corresponds to a maximum time span of ± 20 Ka (thousand years), suggesting that the Allende CAI formation events were culminated within this time span. Although all Allende CAIs studied experienced multistage formation history, including melting and evaporation in the solar nebula and post-crystallization alteration likely on the asteroidal parent body, the 26Al–26Mg and U–Pb-isotopic systematics of the mineral separates and bulk CAIs behaved largely as closed-system since their formation. Our data do not support the “supra-canonical” 26Al/27Al ratio of individual minerals or their mixtures in CV CAIs, suggesting that the supra-canonical 26Al/27Al ratio in the CV CAIs may have resulted from post-crystallization inter-mineral redistribution of Mg isotopes within an individual inclusion. This redistribution must be volumetrically minor in order to satisfy the mass balance of the precisely defined bulk CAI and bulk mineral data obtained by MC-ICP-MS.The radiogenic 208Pb/206Pb ratio obtained as a by-product from the Pb–Pb age dating is used to estimate time-integrated 232Th/238U ratio (κ value) of CAIs. Limited κ variations among the minerals within a single CAI, contrasted by much larger variations among the bulk CAIs, suggest Th/U fractionation occurred prior to crystallization of igneous CAIs. If interpreted as primordial heterogeneity, the κ value can be used to calculate the mean age of the interstellar dust from which the CAIs condensed.  相似文献   

6.
A Porites sp. coral growing offshore from the Sepik and Ramu Rivers in equatorial northern Papua New Guinea has yielded an accurate 20-year history (1977–1996) of sea surface temperature (SST), river discharge, and wind-induced mixing of the upper water column. Depressions in average SSTs of about 0.5–1.0 °C (indicated by coral Sr/Ca) and markedly diminished freshwater runoff to the coastal ocean (indicated by coral δ18O, δ13C and UV fluorescence) are evident during the El Niño – Southern Oscillation (ENSO) events of 1982–1983, 1987 and 1991-1993. The perturbations recorded by the coral are in good agreement with changes in instrumental SST and river discharge/precipitation records, which are known to be diagnostic of the response of the Pacific Warm Pool ocean–atmosphere system to El Niño. Consideration of coastal ocean dynamics indicates that the establishment of northwest monsoon winds promotes mixing of near-surface waters to greater depths in the first quarter of most years, making the coral record sensitive to changes in the Asian–Australian monsoon cycle. Sudden cooling of SSTs by 1°C following westerly wind episodes, as indicated by the coral Sr/Ca, is consistent with greater mixing in the upper water column at these times. Furthermore, the coral UV fluorescence and oxygen isotope data indicate minimal contribution of river runoff to surface ocean waters at the beginning of most years, during the time of maximum discharge. This abrupt shift in flood-plume behaviour appears to reflect the duration and magnitude of northwest monsoon winds, which tend to disperse flood plume waters to a greater extent in the water column when wind-mixing is enhanced. Our results suggest that a multi-proxy geochemical approach to the production of long coral records should provide comprehensive reconstructions of tropical paleoclimate processes operating on interannual timescales.  相似文献   

7.
Uranium-series dating is a critical tool in quaternary geochronology, including paleoclimate work, archaeology and geomorphology. Laser ablation (LA) methods are not as precise as most isotope dilution methods, but can be used to generate calendar ages rapidly, expanding the range of dating tools that can be applied to late Pleistocene carbonates. Here, existing LA methods are revisited for corals (cold- and warm-water) and speleothems spanning the last 343 thousand years (ka). Measurement of the required isotopes (238U, 234U, 230Th and 232Th) is achieved by coupling a laser system to a multi-collector inductively-coupled-plasma mass spectrometer (MC-ICPMS) using a combination of a single central ion counter and an array of Faraday cups. Each sample analysis lasts for ∼4.3 min, and fifty samples can be measured in 12 h with an automated set up, after a day of sample preparation. The use of different standard materials and laser systems had no significant effect on method accuracy. Uncertainty on the measured (230Th/238U) activity ratios ranges from 5.4% to 7.6% for (230Th/238U) ratios equal to 0.7 and 0.1 respectively. Much of this uncertainty can be attributed to the heterogeneity of the standard material (230Th/238U) at the length scale of LA. A homogeneous standard material may therefore improve measurement uncertainty but is not a requirement for age-screening studies. The initial (234U/238U) of coral samples can be determined within ∼20‰, making it useful as a first indicator of open-system behaviour. For cold-water corals, success in determination of (232Th/238U) – which can affect final age accuracy – by LA depended strongly on sample heterogeneity. Age uncertainties (2 sigma) ranged from <0.8 ka at 0–10 ka, ∼1.5 ka at 20 ka to ∼15 ka at 125 ka. Thus, we have demonstrated that U-series dating by LA-MC-ICPMS can be usefully applied to a range of carbonate materials as a straightforward age-screening technique.  相似文献   

8.
The geochronology of cave deposits in the Cradle of Humankind UNESCO World Heritage Site in South Africa provides a timeframe essential for the interpretation of its fossils. The uranium-lead (U–Pb) and uranium-thorium disequilibrium (U/Th) dating of speleothems, mostly flowstones that underlie and blanket the fossil-bearing sediments, have been effective in this sense, but U–Pb is limited by the requirement of ∼1 ppm U concentrations and low common Pb contents, and U/Th has a c. 500 ka limit of applicability. Here we report age results for calcite-aragonite speleothems obtained using a new combined uranium-thorium-helium ((U,Th)–He) and U/Th dating routine. We reproduced within analytical uncertainty, the published U–Pb or U/Th ages for (a) flowstone in three drill core samples in the range 2000–3000 ka, (b) a flowstone hand sample taken at surface with an age of 1800 ka, and (c) five underground flowstone samples in the range 100–800 ka. Calcite retentivity for He under cave conditions is thus demonstrated. In the few cases where helium loss was observed in speleothems, only some of the subsamples were affected, and to varying degrees, suggesting loss by lattice damage not related to diagenetic processes, rather than volume diffusion. In the 100 to 800 ka range, the combined U/Th disequilibrium and (U,Th)–He method also yielded reliable values for initial (230Th/238U) and (234U/238U) activity ratios. Importantly, most subsamples had high initial (230Th/238U) values, ranging from 1.0 to 19.7, although having low Th/U ratios. This is probably due to incorporation of Fe–Mn oxides-hydroxides dust, on which 230Th was previously adsorbed. Such samples are mostly not dateable by U/Th without the additional input from the He analysis. If not detected and corrected for, such high initial (230Th/238U) values can lead to inaccurate U/Th and U–Pb ages. Our study shows that the incorporation of He analysis in U/Th dating has broad potential application, with four methods for calculating the ages, in carbonates from different environments where U-Pb or U/Th dating would not work.  相似文献   

9.
Uranium-series dating of pedogenic carbonate crusts from fluvial gravels is tested using Optically Stimulated Luminescence (OSL) ages as references. OSL dating yielded ages of 30–15 ka and 13–11 ka, which correlate with the cold periods of the Last Glacial Maximum and the Younger Dryas. These ages are internally coherent and consistent with the geological background and are thus regarded as reliable. Most of the U/Th results scatter widely in the 230Th/232Th vs. 234U/232Th isochron diagram, making regression unrealistic. Semiquantitative age estimates from the data were found to be mostly older than the OSL ages and the geological context. It is suggested that a heterogeneous initial 230Th input, not relatable to a detrital component, is responsible for the observed discrepancies. This input may be due to bacterial activities and Th transport on organic colloids. It appears necessary to avoid samples where bacteria could have contributed to carbonate precipitation. Further, the relative importance of this problem decreases with sample age, so that U/Th dating of sinters is expected to be more reliable in the >100 ka age range.  相似文献   

10.
We have studied two young speleothems, SC4 from Smiths Cave (Christmas Island, eastern Indian Ocean) and WM7 from Wollondilly Cave (Wombeyan caves, SE Australia). Attempts to date these speleothems by the Th/U method have proved unsuccessful with some age reversals for SC4 due to multiple sources of non-authigenic Th. This method has also resulted in imprecise ages for WM7 because of low U concentrations (<10 ppb) and consequently very low levels of authigenic 230Th relative even to the very low levels of detrital 230Th present. Here, we present an alternative method for reliable dating of these young speleothems using radiocarbon. Approximately 100 carbonate samples from SC4 and WM7 were analysed for 14C by accelerator mass spectrometry (AMS). The AMS results indicate that bomb 14C was evident in the youngest parts of both stalagmites. Two different approaches were used to estimate dead carbon fraction (DCF) values for these stalagmites for the pre-bomb period. For SC4, the DCF values were estimated based on the timing of 14C dates for that period determined by high-resolution δ18O recorded in the speleothem, and the timing of the onset of bomb 14C. For WM7, a “maximum” range of pre-bomb DCF was determined. Chronologies of these speleothems were built based on a dense sequence of DCF-corrected ages using three different age-depth models: Clam (Classical method), and Bacon and OxCal (Bayesian statistical approach). Good agreement between these age-depth models were observed indicating that the top 170 mm of SC4 and the top 50 mm of WM7 grew during the past 550–750 years and 1360–1740 years, respectively.  相似文献   

11.
Recently, alternative models to estimate the age of diagenetically altered fossil reef corals have been presented based on either redistribution of U or its immediate daughters 234Th and 230Th. Here, we present three methods to estimate the uncertainty of ages derived using an amended version of our coral isochron method [Scholz et al., 2004. U-series dating of diagenetically altered fossil reef corals. Earth and Planetary Science Letters 218, 163–178], which is based on addition/loss of U. The obtained uncertainties are substantially larger than those previously published and should, in general, be more reliable. The isochron method yields larger uncertainties than alternative models based on Th redistribution due to -recoil processes. However, comparison of model open-system ages based on such redistribution of U-series daughters for different sub-samples from an individual coral specimen shows that the smaller errors derived with these models cannot account for the observed variability. We recognise that none of the available models is applicable to all corals, probably reflecting different diagenetic processes even in different sub-samples from one coral specimen. To better understand the diagenetic processes and precisely constrain the uncertainties of the ages derived from diagenetically altered corals, the application of all available models is recommended.  相似文献   

12.
Silica chimneys were discovered in 1985 at 86°W in the rift valley of the Galapagos Spreading Center at 2600 m depth (“Cauliflower Garden”). The inactive chimneys lack any sulfides and consist almost entirely of amorphous silica (up to 96 wt.% SiO2, opal-A); Fe and Mn oxides are minor constituents. Oxygen isotope data show that formation of the silica chimneys took place at temperatures between 32°C (+29.9‰ δ18O) and 42°C (+27.8‰ δ18O).Th/Udating reveals a maximum age of 1440 ± 300y. Amorphous silica solubility relations indicate that the silica chimneys were formed by conductive cooling of pure hydrothermal fluids or by conductive cooling of a fluid/seawater mixture. Assuming equilibrium with quartz at 500 bars, initial fluid temperatures of more than 175°C (i.e., a concentration of > 182 ppm SiO2) were required to achieve sufficient supersaturation for the deposition of amorphous silica at 40°C and 260 bars. If the silica chimneys originate from the same or a similar fluid as higher-temperature ( < 300°C) sulfide-silica precipitates found nearby (i.e., 2.5 km away), then subsurface deposition of sulfides may have occurred.  相似文献   

13.
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14.
Uranium-series ages have been obtained for 87 speleothems collected from nine major cave systems in the Craven district of northern England. Large systems such as Ease Gill Caverns, the West Kingsdale caves, and Gaping Gill-Ingleborough Cave, which contain relict high-level tunnels, are found to be older than 350,000 years (the limit of the 230Th/234U dating method). There is little evidence to indicate a significant enlargement of these passages since this time. Estimates of the age of Victoria Cave from 234U/238U isotopic ratios suggest that the cave has been fully relict for more than 500,000 years. Ages of in situ speleothems immediately adjacent to local base level cave streams show that mean maximum downcutting rates in limestone channels are about 2 to 5 cm 1000 yr. These rates are significantly lower than those obtained from direct measurements on limestone bedrock in stream channels but are comparable to areal denudation rates based on solute budgets. Using the present elevation of caves with respect to adjacent valley floor levels, mean maximum valley entrenchment rates are found to range between 5 cm/ky and < 20cm/ky, which corresponds to 6 m to < 24 m of lowering per glacial/interglacial cycle. These rates suggest that upper beds of the limestone were incised to form the Yorkshire Dales between 1 and 2 million years ago. The results indicate that the erosional effects of individual glaciations are not as severe as previously proposed in the literature.  相似文献   

15.
D/H ratios of fluid inclusion waters extracted from230Th/234U-dated speleothems that were originally deposited under conditions of isotopic equilibrium should provide a direct estimate of the hydrogen isotopic composition of ancient meteoric waters. We present here D/H ratios for 47 fluid inclusion samples from thirteen speleothems deposited over the past 250,000 years at cave sites in Iowa, West Virginia, Kentucky and Missouri. At each site glacial-age waters are depleted in deuterium relative to those of interglacial age. The average interglacial/glacial shift in the hydrogen isotopic composition of meteoric precipitation over ice-free areas of east-central North America is estimated to be ?12‰. This shift is consistent with the present climatic models and can be explained in terms of the prevailing pattern of atmospheric circulation and an increased ocean-continent temperature gradient during glacial times which more than compensated for the increase in deuterium content of the world ocean.  相似文献   

16.
Correct and precise age determination of prehistorical catastrophic rock‐slope failures prerequisites any hypotheses relating this type of mass wasting to past climatic regimes or palaeo‐seismic records. Despite good exposure, easy accessibility and a long tradition of absolute dating, the age of the 230 million m3 carbonate‐lithic Tschirgant rock avalanche event of the Eastern Alps (Austria) still is relatively poorly constrained. We herein review the age of mass‐wasting based on a total of 17 absolute ages produced with three different methods (14C, 36Cl, 234U/230Th). Chlorine‐36 (36Cl) cosmogenic surface exposure dating of five boulders of the rock avalanche deposit indicates a mean event age of 3.06 ± 0.62 ka. Uranium‐234/thorium‐230 (234U/230Th) dating of soda‐straw stalactites formed in microcaves beneath boulders indicate mean precipitation ages of three individual soda straws at 3.20 ± 0.26 ka, 3.04 ± 0.10 ka and 2.81 ± 0.15 ka; notwithstanding potential internal errors, these ages provide an ‘older‐than’ (ante quam) proxy for mass‐wasting. Based on radiocarbon ages (nine sites) only, it was previously suggested that the present rock avalanche deposit represents two successive failures (3.75 ± 0.19 ka bp , 3.15 ± 0.19 ka bp ). There is, however, no evidence for two events neither in surface outcrops nor in LiDAR derived imagery and drill logs. The temporal distribution of all absolute ages (14C, 36Cl, 234U/230Th) also does not necessarily indicate two successive events but suggest that a single catastrophic mass‐wasting took place between 3.4 and 2.4 ka bp . Taking into account the maximum age boundary given by reinterpreted radiocarbon datings and the minimum U/Th‐ages of calcite precipitations within the rock avalanche deposits, a most probable event age of 3.01 ± 0.10 ka bp can be proposed. Our results underscore the difficulty to accurately date catastrophic rock slope failures, but also the potential to increase the accuracy of age determination by combining methods. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

17.
Basic properties of the mid-latitude traveling ionospheric disturbances (TIDs) during the maximum phase of a major magnetic storm of 6–8 April 2000 are shown. Total electron content (TEC) variations were studied by using data from GPS receivers located in Russia and Central Asia. The nightglow response to this storm at mesopause and termospheric altitudes was also measured by optical instruments FENIX located at the observatory of the Institute of Solar-Terrestrial Physics (51.9°N,103.0°E), and MORTI located at the observatory of the Institute of Ionosphere (43.2°N, 77.0°E). Observations of the O (557.7 and 630.0 nm) emissions originating from atmospheric layers centered at altitudes of 90 and 250 km were carried out at Irkutsk and of the O2(b1∑g+−X3∑g−) (0-1) emission originating from an atmospheric layer centered at altitude of 94 km was carried out at Almaty. Our radio and optical measurement network observed a storm-induced solitary large-scale wave with duration of 1 h and a wave front width of no less than 5000 km, while it traveled equatorward with a velocity of 200 m/s from 62°N to 38°N geographic latitude. The TEC disturbance, basically displaying an electron content depression in the maximum of the F2 region, reveals a good correlation with growing nightglow emission, the temporal shift between the TEC and emission variation maxima being different for different altitudes. A comparison of the auroral oval parameters with dynamic spectra of TEC variations and optical 630 nm emissions in the frequency range 0.4–4 mHz (250–2500 s periods) showed that as the auroral oval expands into mid-latitudes, also does the region with a developed medium-sale and small-scale TEC structure.  相似文献   

18.
From previously published 14C and K–Ar data, the age of formation of Lake Nyos maar in Cameroon is still in dispute. Lake Nyos exploded in 1986, releasing CO2 that killed 1750 people and over 3000 cattle. Here we report results of the first measurements of major elements, trace elements and U-series disequilibria in ten basanites/trachy-basalts and two olivine tholeiites from Lake Nyos. It is the first time tholeiites are described in Lake Nyos. But for the tholeiites which are in 238U–230Th equilibrium, all the other samples possess 238U–230Th disequilibrium with 15 to 28% enrichment of 230Th over 238U. The (226Ra/230Th) activity ratios of these samples indicate small (2 to 4%) but significant 226Ra excesses. U–Th systematics and evidence from oxygen isotopes of the basalts and Lake Nyos granitic quartz separates show that the U-series disequilibria in these samples are source-based and not due to crustal contamination or post-eruptive alteration. Enrichment of 230Th is strong prima facie evidence that Lake Nyos is younger than 350 ka. The 230Th–226Ra age of Nyos samples calculated with the (226Ra/230Th) ratio for zero-age Mt. Cameroon samples is 3.7 ± 0.5 ka, although this is a lower limit as the actual age is estimated to be older than 5 ka, based on the measured mean 230Th/238U activity ratio. The general stability of the Lake Nyos pyroclastic dam is a cause for concern, but judging from its 230Th–226Ra formation age, we do not think that in the absence of a big rock fall or landslide into the lake, a big earthquake or volcanic eruption close to the lake, collapse of the dam from erosion alone is as imminent and alarming as has been suggested.  相似文献   

19.
We have used in-situ pumps which filter large volumes of sea water through a 1 μm cartridge prefilter and two MnO2-coated cartridges to obtain information on dissolved and particulate radionuclide distributions in the oceans. Two sites in the northwest Atlantic show subsurface maxima of the fallout radionuclides137Cs,239,240Pu and241Am. Although the processes of scavenging onto sinking particles and release at depth may contribute to the tracer distributions, comparison of predicted and measured water column inventories suggests that at least 35–50% of the Pu and241Am are supplied to the deep water by advection.The depth distributions of the naturally occurring radionuclides232Th,228Th and230Th reflect their sources to the oceans.232Th shows high dissolved concentrations in surface waters, presumably as a result of atmospheric or riverine supply. Activities of232Th decrease with depth to values 0.01 dpm/1000 l.228Th shows high activities in near surface and near bottom water, due to the distribution of its parent,228Ra. Dissolved230Th, produced throughout the water column from234U decay, increases with depth to 3000 m. Values in the deep water (> 3000 m) are nearly constant ( 0.6–0.7 dpm/1000 l), and the distribution of this tracer (and perhaps other long-lived particle-reactive tracers as well) may be affected by the advection inferred from Pu and241Am data.The ratio of particulate to dissolved activity for both230Th and228Th is 0.15–0.20. This similarity precludes the calculation of sorption rate constants using a simple model of reversible sorption equilibrium. Moreover, in mid-depths228Th tends to have a higher particulate/dissolved ratio than230Th, suggesting uptake and release of230Th and228Th by different processes. This could occur if228Th, produced in surface water, were incorporated into biogenic particles formed there and released as those particles dissolved or decomposed during sinking.230Th, produced throughout the water column, may more closely approach a sorption equilibrium at all depths.230Th,241Am and239,240Pu are partitioned onto particles in the sequence Th > Am > Pu with 15% of the230Th on particles compared with 7% for Am and 1% for Pu. Distribution coefficients (Kd) are 1.3–1.6 × 107 for Th, 5–6 × 106 for Am and 7–10 × 105 for Pu. The lower reactivity for Pu is consistent with analyses of Pu oxidation states which show 85% oxidized (V + VI) Pu. However, theKd value for Pu may be an upper limit because Pu, like228Th, may be incorporated into particles in surface waters and released at depth only by destruction of the carrier phase.  相似文献   

20.
Samples from Kawah Ijen crater lake, spring and fumarole discharges were collected between 1990 and 1996 for chemical and isotopic analysis. An extremely low pH (<0.3) lake contains SO4–Cl waters produced during absorption of magmatic volatiles into shallow ground water. The acidic waters dissolve the rock isochemically to produce “immature” solutions. The strong D and 18O enrichment of the lake is mainly due to enhanced evaporation at elevated temperature, but involvement of a magmatic component with heavy isotopic ratios also modifies the lake D and 18O content. The large ΔSO4–S0 (23.8–26.4‰) measured in the lake suggest that dissolved SO4 forms during disproportionation of magmatic SO2 in the hydrothermal conduit at temperatures of 250280°C. The lake δ18OSO4 and δ18OH2O values may reflect equilibration during subsurface circulation of the water at temperatures near 150°C. Significant variations in the lake's bulk composition from 1990 to 1996 were not detected. However, we interpret a change in the distribution and concentration of polythionate species in 1996 as a result of increased SO2-rich gas input to the lake system.Thermal springs at Kawah Ijen consist of acidic SO4–Cl waters on the lakeshore and neutral pH HCO3–SO4–Cl–Na waters in Blawan village, 17 km from the crater. The cation contents of these discharges are diluted compared to the crater lake but still do not represent equilibrium with the rock. The SO4/Cl ratios and water and sulfur isotopic compositions support the idea that these springs are mixtures of summit acidic SO4–Cl water and ground water.The lakeshore fumarole discharges (T=170245°C) have both a magmatic and a hydrothermal component and are supersaturated with respect to elemental sulfur. The apparent equilibrium temperature of the gas is 260°C. The proportions of the oxidized, SO2-dominated magmatic vapor and of the reduced, H2S-dominated hydrothermal vapor in the fumaroles varied between 1979 and 1996. This may be the result of interaction of SO2-bearing magmatic vapors with the summit acidic hydrothermal reservoir. This idea is supported by the lower H2S/SO2 ratio deduced for the gas producing the SO4–Cl reservoir feeding the lake compared with that observed in the subaerial gas discharges. The condensing gas may have equilibrated in a liquid–vapor zone at about 350°C.Elemental sulfur occurs in the crater lake environment as banded sediments exposed on the lakeshore and as a subaqueous molten body on the crater floor. The sediments were precipitated in the past during inorganic oxidation of H2S in the lake water. This process was not continuous, but was interrupted by periods of massive silica (poorly crystallized) precipitation, similar to the present-day lake conditions. We suggest that the factor controlling the type of deposition is related to whether H2S- or silica-rich volcanic discharges enter the lake. This could depend on the efficiency with which the lake water circulates in the hydrothermal cell beneath the crater. Quenched liquid sulfur products show δ34S values similar to those found in the banded deposits, suggesting that the subaqueous molten body simply consists of melted sediments previously accumulated at the lake bottom.  相似文献   

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