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1.
We present U, Th, and Pa isotope data for young lavas from Costa Rica and Nicaragua in the Central American arc. Thorium isotopic ratios for Costa Rica and Nicaragua differ dramatically: Costa Rican lavas are characterized by low (230Th/232Th) (1 to 1.2) and, for four out of five lavas, (230Th/238U) greater than unity. Nicaraguan lavas have high (230Th/232Th) (2.2 to 2.7) and, for five of six samples, (230Th/238U) less than unity. All lavas have (231Pa/235U) greater than unity, with initial values ranging from 1.27 to 1.77, but those from Costa Rica have larger 231Pa excesses. There is a broad positive correlation between (231Pa/235U) and (230Th/238U) similar to the worldwide trend for arcs outlined by Pickett and Murrell (1997), although many of the Nicaraguan lavas skirt the high end of that trend. In greater detail, the Central American data appear to divide into separate high-(231Pa/235U) and low-(231Pa/235U) tiers. These tiers may be different because of either different residence times in the crust or different proportions of sedimentary components from the slab.Substantial (231Pa/235U) excesses (>1.5) in both Costa Rica and Nicaragua require a melting process that allows for enhanced daughter (231Pa) ingrowth. With increasing U addition, (231Pa/230Th) increases in a manner that cannot be explained adequately by aging of fluid components before partial melting and eruption. Thus, either some 231Pa is added from the slab, or melting-enhanced 231Pa ingrowth is greater in sources that have experienced a larger amount of slab-derived flux and a higher extent of melting. These observations can be explained if regions that have undergone greater extents of fluxing and melting have experienced these processes over a longer time interval than those that have had little flux added and little melt extracted. We propose a flux-ingrowth melting model in which corner flow in the mantle wedge supplies fresh hot mantle into a zone of slab fluid addition. Partial melting occurs in response to this fluxing. We assume critical melting at low porosity (∼10−3), rapid fluid flux to the melting region, and rapid melt transport. Solid mantle traverses the melting region over 105 to 106 yr, thereby allowing 231Pa and 230Th ingrowth from U retained in the residues of melt extraction. Magmas are aggregated from all parts of the melting regime, mixing melts from incipiently fluxed regions with those from sources that have experienced more extensive fluid addition, partial melting, and daughter nuclide ingrowth. With suitable assumptions about component addition from the slab, this flux-ingrowth model matches a wide range of U-series and trace element data from Costa Rican and Nicaraguan lavas, with required average extents of melting of ∼1 to 3% and 7 to 15%, respectively. Upwelling and/or extensive melt-rock reaction are not required to explain large (231Pa/235U) excesses in Central America or other arcs. On Th isotope equiline plots, the model produces linear arrays that resemble isochrons but that have no age significance. Instead, these arrays are generated by mixing of melts from sources that have experienced fluid addition and partial melting over a range of time intervals, as seems likely in arc source regions. Finally, the flux-ingrowth model predicts considerable 226Ra excesses for integrated magmas. If we assume that 226Ra is added continuously with the slab-derived fluid, the model predicts large and increasing (226Ra/230Th) with increasing melting and slab-component addition, without requiring the addition of a distinct late fluid.  相似文献   

2.
To examine the petrogenesis and sources of basalts from the Kolbeinsey Ridge, one of the shallowest locations along the global ridge system, we present new measurements of Nd, Sr, Hf, and Pb isotopes and U-series disequilibria on 32 axial basalts. Young Kolbeinsey basalts (full-spreading rate = 1.8 cm/yr; 67°05′-70°26′N) display (230Th/238U) < 1 and (230Th/238U) > 1 with (230Th/238U) from 0.95 to 1.30 and have low U (11.3-65.6 ppb) and Th (33.0 ppb-2.40 ppm) concentrations. Except for characteristic isotopic enrichment near the Jan Mayen region, the otherwise depleted Kolbeinsey basalts (e.g. 87Sr/86Sr = 0.70272-0.70301, εNd = 8.4-10.5, εHf = 15.4-19.6 (La/Yb)N = 0.28-0.84) encompass a narrow range of (230Th/232Th) (1.20-1.32) over a large range in (238U/232Th) (0.94-1.32), producing a horizontal array on a (230Th/232Th) vs. (238U/232Th) diagram and a large variation in (230Th/238U). However, the (230Th/238U) of the Kolbeinsey Ridge basalts (0.96-1.30) are inversely correlated with (234U/238U) (1.001-1.031). Samples with low (230Th/238U) and elevated (234U/238U) reflect alteration by seawater or seawater-derived materials. The unaltered Kolbeinsey lavas with equilibrium 234U/238U have high (230Th/238U) values (?1.2), which are consistent with melting in the presence of garnet. This is in keeping with the thick crust and anomalously shallow axial depth for the Kolbeinsey Ridge, which is thought to be the product of large degrees of melting in a long melt column. A time-dependent, dynamic melting scenario involving a long, slowly upwelling melting column that initiates well within the garnet peridotite stability zone can, in general, reproduce the (230Th/238U) and (231Pa/235U) ratios in uncontaminated Kolbeinsey lavas, but low (231Pa/235U) ratios in Eggvin Bank samples suggest eclogite involvement in the source for that ridge segment.  相似文献   

3.
We present data for U and its decay series nuclides 230Th, 226Ra, 231Pa, and 210Po for 14 lavas from Kick’em Jenny (KEJ) submarine volcano to constrain the time-scales and processes of magmatism in the Southern Lesser Antilles, the arc having the globally lowest plate convergence rate. Although these samples are thought to have been erupted in the last century, most have (226Ra)/(210Po) within ±15% of unity. Ten out of 14 samples have significant 226Ra excesses over 230Th, with (226Ra)/(230Th) up to 2.97, while four samples are in 226Ra-230Th equilibrium within error. All KEJ samples have high (231Pa)/(235U), ranging from 1.56 to 2.64 and high 238U excesses (up to 43%), providing a global end-member of high 238U and high 231Pa excesses. Negative correlations between Sr, sensitive to plagioclase fractionation, and Ho/Sm, sensitive to amphibole fractionation, or K/Rb, sensitive to open system behavior, indicate that differentiation at KEJ lavas was dominated by amphibole fractionation and open-system assimilation. While (231Pa)/(235U) does not correlate with differentiation indices such as Ho/Sm, (230Th)/(238U) shows a slight negative correlation, likely due to assimilation of materials with slightly higher (230Th)/(238U). Samples with 226Ra excess have higher Sr/Th and Ba/Th than those in 226Ra-230Th equilibrium, forming rough positive correlations of (226Ra)/(230Th) with Sr/Th and Ba/Th similar to those observed in many arc settings. We interpret these correlations to reflect a time-dependent magma differentiation process at shallow crustal levels and not the process of recent fluid addition at the slab-wedge interface.The high 231Pa excesses require an in-growth melting process operating at low melting rates and small residual porosity; such a model will also produce significant 238U-230Th and 226Ra-230Th disequilibrium in erupted lavas, meaning that signatures of recent fluid addition from the slab are unlikely to be preserved in KEJ lavas. We instead propose that most of the 238U-230Th, 226Ra-230Th, and 235U-231Pa disequilibria in erupted KEJ lavas reflect the in-growth melting process in the mantle wedge (reflecting variations in U/Th, daughter-parent ratios, fO2, and thermal structure), followed by modification by magma differentiation at crustal depths. Such a conclusion reconciles the different temporal implications from different U-series parent-daughter pairs and relaxes the time constraint on mass transfer from slab to eruption occurring in less than a few thousand years imposed by models whereby 226Ra excess is derived from the slab.  相似文献   

4.
U-series disequilibria are presented for Holocene samples from the Canary Islands and interpreted with special emphasis on the separate roles of plume vs. lithospheric melting processes. We report Th and U concentrations and (238U)/(232Th), (230Th)/(232Th), (230Th)/(238U) and (234U)/(238U) for 43 samples, most of which are minimally differentiated, along with (226Ra)/(230Th) and (231Pa)/(235U) for a subset of these samples, measured by thermal ionization mass spectrometry (TIMS). Th and U concentrations range between 2 and 20 ppm and 0.5 and 6 ppm, respectively. Initial (230Th)/(238U) ranges from 1.1 to 1.6. (226Ra)/(230Th)o ranges between 0.9 and 1.8 while (231Pa)/(235U)o ranges between 1.0 and 2.0.Our interpretation of results is based on a three-fold division of samples as a function of incompatible element ratio, such as Nb/U. The majority of samples have Nb/U = 47 ± 10, similar to most MORB and OIB. Higher ratios are found exclusively in alkali basalts and tholeiites from the eastern Canary Islands whereas lower ratios are exclusively found in differentiated rocks from the western Canary Islands. Those with ordinary Nb/U ratios are attributed to melting within the slowly ascending HIMU-dominated Canary plume.Higher Nb/U, generally found in more silica rich basalts from the eastern islands, is attributed to lithospheric contamination. Based on their trace element characteristics, two possible contaminants are amphibole veins (± other minerals) crystallized in the mantle from previous plume-derived basanite or re-melted plume-derived intrusive rocks. The high Nb/U signature of these materials is imparted on a melt of the lithosphere created either by the diffusive infiltration of alkalis or by direct reaction between basanites and peridotite. Mixing between plume-derived basanite and lithospheric melt accounts for the U-series systematics of most eastern island magmas including the well-known Timanfaya eruption. Lower Nb/U ratios in differentiated rocks from the western islands are attributed to fractional crystallization of amphibole ± phlogopite ± sphene from basanite during its ascent through the lithosphere. Based on changes in disequilibria, phonolites and tephrites are interpreted to result from rapid differentiation of primitive parents within millennia.  相似文献   

5.
Changes in the geomagnetic field intensity, solar variability, and the internal changes of the carbon cycle are believed to be the three controlling factors of past atmospheric radiocarbon (14C) concentrations (denoted as Δ14C). Of these three, it is believed that the field intensity is the dominant factor. We analyze an atmospheric Δ14C record spanning the past 50,000 years based on previously-published 230Th/234U/238U and 14C dates of fossil corals from Kiritimati, Barbados, Araki and Santo Islands, and identify the role of the Laschamp geomagnetic field excursion on the long term trend of the Δ14C record. There is a general consistency between the coral Δ14C record and the Δ14C output from carbon cycle models based on the global 14C production estimates. High-precision, high-accuracy 230Th/234U/238U dates and redundant 231Pa/235U dates anchor the timing of this Δ14C record. We propose that a significant fraction of the long-term Δ14C trend may be due to inaccuracies in the generally accepted 14C decay constant. The uncertainty in estimating the shape of 14C beta spectrum below 20 keV leads to one of the greatest errors in decay constant estimates. Once the 14C half-life is validated via redundant techniques, Δ14C records will provide a better opportunity to examine the roles of carbon cycle and 14C production influences.  相似文献   

6.
The short residence times of Th and Pa in seawater make them very responsive to changes in the ocean environment. We use a new multi-ion-counting technique to make Th and Pa isotope measurements in seawaters from a near-shore environment in which oceanic chemical tracers are not overwhelmed by terrestrial inputs (the Bahamas). An unusual feature of the Bahamas setting is the shallow depth of water residing on the bank tops. These waters have significantly lower 232Th/230Th (∼10,000) than those immediately adjacent to the banks (24,000-31,000) and a (231Pa/230Th) near the production ratio (∼0.1). The change in 232Th/230Th and (231Pa/230Th) on the bank tops is explained by almost quantitative removal of Th and Pa by scavenging, and their replacement with a mixture of 230Th and 231Pa alpha-recoiled from the underlying carbonates, together with Th from dust dissolution. Analysis of a water profile in the Tongue of the Ocean, which separates the Great and Little Bahama Banks, allows us to trace the movement of bank-top water to depth. A distinct minimum in both 232Th/230Th (∼13,000) and (231Pa/230Th) (∼0.5) is observed at ∼430 m and is interpreted to reflect density cascading of bank-top water with entrained carbonate sediment. These results suggest that Th and Pa can be used as water-mass tracers in near-shore environments. Uranium concentration measurements on the same waters demonstrate that U is conservative across a range in salinity of 2 psu, with a concentration of 3.33 ppb (at a salinity of 35).The incorporation of U and Th isotopes into marine carbonates has also been assessed by analyzing carbonate samples from the same location as these Bahamas waters. Such incorporation is critical for U-Th geochronology. U isotope analyses demonstrate that seawater δ234U averages 146.6 and does not vary by more than 2.5%o, and that carbonates capture this value. Additional high precision measurements (≈±1%o) on modern carbonates confirm that all oceans have identical δ234U. Modern marine carbonates are shown to have 232Th/230Th ratios that reflect the local seawater in which they formed.  相似文献   

7.
The processes involved in the formation and transport of partial melts above subducting plates remain poorly constrained relative to those at mid-ocean ridges. In particular, 238U-230Th-226Ra disequilibria, that might normally be used to constrain melting dynamics, tend to be swamped by the effects of fluid addition from the down-going plate. The 231Pa-235U system provides an exciting exception to this because the highly incompatible nature of Pa means that fractionation and in-growth during partial melting overwrite the effects of fluid U addition. We present 231Pa-235U data on 50 well-characterised lavas from seven subduction zones in order to examine partial melting processes. Measured (231Pa/235U) ratios are all >1 and 15% are >2. Overall (231Pa/235U) shows broad positive correlations with (230Th/238U) and La/Yb and negative trends against Ba/Th and (226Ra/230Th). These systematics can differ from arc to arc but suggest that (231Pa/235U) tends to be higher in sediment-rich arc lavas where the effects of fluid addition are muted and there is less of a 231Pa deficit for melting to overprint. We have explored the effects of decompression melting, frictional drag dynamic melting with and without ageing subsequent to fluid U addition to the wedge as well as flux melting models. Globally, average (231Pa/235U) appears to correlate negatively with convergence rate and so in the numerical models we use the local subduction rate for the rate of matrix flow through the melting zone. Using this assumption and reasonable values for other parameters, the melting models can simulate the overall range of (231Pa/235U) and some of the data trends. However, it is clear that local variations in some parameters, especially source composition and extent of melting, exert a major influence on 231Pa-235U disequilibria. Some data, which lie at a high angle to the modelled trends, may be explained by mixing between small degree hydrous melts formed near the slab and larger degree, decompression melts produced at shallow depth.  相似文献   

8.
In order to determine the geochemical evolution of a freshwater limestone cave system located in central Switzerland (Hell Grottoes at Baar/Zug,) young postglacial tufaceous limestone and travertine precipitates were investigated using the 230Th/234U ingrowth system. Additional analyses of further radionuclides within the 238U decay chain, i.e. 226Ra and 210Pb, showed that the Th/U chronometer started with insignificant inherited 230Th over the entire formation period of the travertine setting (i.e. 230Th(0)=0). A contribution from detrital impurities with 230Th/234U in secular equilibrium could be precisely subtracted by applying isochron dating of cogenetic phases and recently formed travertine. The resulting precise 230Th/234U formation ages were found to be consistent with the geological stratigraphy and were furthermore used to demonstrate the applicability of the next geologically important chronometer in the 238U-decay series, based on decay of excess 226Ra normalized to the initial, i.e.226Raex/226Ra(0). This system is suitable for dating phases younger than 7000 yr when the correction of a detritus component increasingly limits the precision of the 230Th/234U chronometer. Analytical solutions of the coupled 234U/230Th/226Ra radionuclide system predicted that the 226Raex/226Ra(0) chronometer is independent of the actual 230Th activity build up from decay of 234U, if the systems starts with zero inherited 230Th(0). The data set confirmed this hypothesis and showed furthermore that the initially incorporated 226Ra excess must have remained almost uniform in all limestone over a period of at least 7000 yr, i.e. 4–5 half-lives of 226Ra. This is concluded because (i) the 226Raex/226Ra(0) ages agreed well with those derived from 230Th/234U, (ii) all data plot within uncertainty on the 226Raex/226Ra(0) decay curve and (iii) the atomic Ba/Ca ratio was found to be constant in the travertine material independent of the sample ages. Provided that such boundary conditions hold, 226Raex/226Ra(0) should be applicable to materials which are suitable for 230Th/234U dating in sedimentology and oceanography, i.e. travertine, corals, phosphorites, etc., and should strongly support 230Th/234U for samples that have been formed a few thousand years ago.  相似文献   

9.
洞穴地点骨化石铀系年龄可信度的讨论*   总被引:2,自引:1,他引:1  
沈冠军 《第四纪研究》2007,27(4):539-545
骨化石是铀不平衡系测年法广泛应用而又颇有争议的研究对象。文章通过对典型铀加入模式的计算,指出以α能谱的精度,二种铀系年龄差异的显著性表明近期内有较大量铀的迁移,但其在误差范围内的一致不能保证样品构成封闭体系。以往积累的数据表明,大多数洞穴地点骨化石给出了二法一致的铀系年龄,但钙板与下伏骨化石铀系年龄大多差异显著且与地层顺序矛盾,即使被次生碳酸盐岩包裹,多半骨化石的铀系年龄仍显著偏低于其包裹体。此外,相当一部分样品的U-Th同位素比难以用简单的铀后期加入或淋失来解释。基于对次生碳酸盐岩铀系年龄可信度的认识,骨化石总体上不构成封闭体系,所载铀系年代信息只具有限的分辨率。  相似文献   

10.
The 238U-230Th-226Ra and 235U-231Pa disequilibria have been measured by mass spectrometry in historic lavas from the Kamchatka arc. The samples come from three closely located volcanoes in the Central Kamchatka Depression (CKD), the most active region of subducted-related volcanism in the world. The large excesses of 226Ra over 230Th found in the CKD lavas are believed to be linked to slab dehydration. Moreover, the samples show the uncommon feature of (230Th/238U) activity ratios both lower and higher than 1. The U-series disequilibria are characterized by binary trends between activity ratios, with (231Pa/235U) ratios all >1. It is shown that these correlations cannot be explained by a simple process involving a combination of slab dehydration and melting. We suggest that they are more likely to reflect mixing between two end-members: a high-magnesia basalt (HMB) end-member with a clear slab fluid signature and a high-alumina andesite (HAA) end-member reflecting the contribution of a slab-derived melt. The U-Th-Ra characteristics of the HMB end-member can be explained either by a two-step fluid addition with a time lag of 150 ka between each event or by continuous dehydration. The inferred composition for the dehydrating slab is a phengite-bearing eclogite. Equilibrium transport or dynamic melting can both account for 231Pa excess over 235U in HMB end-member. Nevertheless, dynamic melting is preferred as equilibrium transport melting requires unrealistically high upwelling velocities to preserve fluid-derived 226Ra/230Th. A continuous flux melting model is also tested. In this model, 231Pa-235U is quickly dominated by fluid addition and, for realistic extents of melting, this process cannot account for (231Pa/235U) ratios as high as 1.6, as observed in the HMB end-member.The involvement of a melt derived from the subducted oceanic crust is more likely for explaining the HAA end-member compositions than crustal assimilation. Melting of the oceanic crust is believed to occur in presence of residual phengite and rutile, resulting in no 226Ra-230Th disequilibrium and low 231Pa excess over 235U in the high-alumina andesites. Consequently, it appears that high-alumina andesites and high-magnesia basalts have distinct origins: the former being derived from melting of the subducted oceanic crust and the latter from hydrated mantle. It seems that there is no genetic link between these two magma types, in contrast with what was previously believed.  相似文献   

11.
A 230Th-234U-238U dating study on pedogenic silica-carbonate clast rinds and matrix laminae from alluvium in Crater Flat, Nevada was conducted using small-sample thermal-ionization mass spectrometry (TIMS) analyses on a large suite of samples. Though the 232Th content of these soils is not particularly low (mostly 0.1-9 ppm), the high U content of the silica component (mostly 4-26 ppm) makes them particularly suitable for 230Th/U dating on single, 10 to 200 mg totally-digested samples using TIMS. We observed that (1) both micro- (within-rind) and macro-stratigraphic (mappable deposit) order of the 230Th/U ages were preserved in all cases; (2) back-calculated initial 234U/238U fall in a restricted range (typically 1.67±0.19), so that 234U/238U ages with errors of about 100 kyr (2σ) could be reliably determined for the oldest, 400 to 1000 ka rinds; and (3) though 13 of the samples were >350 ka, only three showed evidence for an open-system history, even though the sensitivity of such old samples to isotopic disruption is very high. An attempt to use leach-residue techniques to separate pedogenic from detrital U and Th failed, yielding corrupt 230Th/U ages. We conclude that 230Th/U ages determined from totally dissolved, multiple sub-mm size subsamples provide more reliable estimates of soil chronology than methods employing larger samples, chemical enhancement of 238U/232Th, or isochrons.  相似文献   

12.
研究了TIMS测定铀矿石样品中234U/238U、230Th/232Th、228Ra/226Ra的方法。建立了铀矿石密闭混酸一次溶样的方法和采用阴离子、阳离子和Sr特效树脂逐级离子交换分离纯化U、Th和Ra的流程,满足了TIMS测量要求。测定结果表明:100~1000 ng的天然铀中234U/238U,其测量精密度从静态多接收的2.34%提高到动态多接收的0.47%;对230Th与232Th丰度接近、质量为1μg左右的钍,采用三带点样技术和法拉第多接收技术测定230Th/232Th,其内精度平均值为0.0048%,外精度为0.028%;采用单带加钽发射剂,ETP跳峰测定50~100 fg镭-228稀释剂中的228Ra/226Ra,其内精度小于0.10%,外精度小于0.20%。比较TIMS和HR-ICP-MS、α能谱法测定234U/238U、230Th/232Th、228Ra/226Ra结果,三者结果相吻合。TIMS测量法样品用量少、快速、准确、精密度高,是U、Th、Ra同位素比值测定方法的又一补充。  相似文献   

13.
We present the results of a comparative study of several geochronometer minerals (baddeleyite, zircon, apatite, phlogopite and tetraferriphlogopite) and isotopic systems (U-Pb, Th-Pb and Rb-Sr) from phoscorites (magnetite-forsterite-apatite-calcite rocks) and carbonatites of the Kovdor ultramafic-alkaline-carbonatite massif, Kola Peninsula, Russia. Uranium, thorium and their decay products are extremely fractionated by minerals that crystallise from carbonatite and phoscorite magma. We obtain high-precision ages from different chronometers, compare their accuracy, and evaluate the role of geochronological pitfalls of initial radioactive disequilibrium, differential migration of radiogenic isotopes, and inaccurate decay constants.Apatite yielded concordant U-Th-Pb ages between 376 and 380 Ma. The accuracy of the apatite 238U-206Pb ages is, however, compromised by uncertainty in the amount of radiogenic 206Pb produced from initial excess 230Th. The 235U-207Pb ages are relatively imprecise due to large common Pb correction and the uncertainty in the initial Pb isotopic composition. The Th-Pb system yields a more precise age of 376.4 ± 0.6 Ma.Zircon from two carbonatite samples is characterised by moderate to low U contents, high Th contents, and very high Th/U ratios up to 9000. The 206Pb*/238U systems in the zircon are strongly affected by the presence of excess 206Pb*, produced by decay of initial 230Th. The 208Pb*/232Th ages of zircon from both carbonatite samples are uniform and yield a weighted average of 377.52 ± 0.94 Ma.Baddeleyite U-Pb analyses are 3 to 6% normally discordant and have variable 207Pb*/206Pb* apparent ages. Eleven alteration-free baddeleyite fractions from three samples with no evidence for Pb loss yield uniform 206Pb*/238U ages with a weighted average of 378.54±0.23 Ma (378.64 Ma after correction for initial 230Th deficiency), which we consider the best estimate for age of the phoscorite-carbonatite body of the Kovdor massif. The 206Pb*/238U ages of baddeleyite fractions from five other samples spread between 378.5 and 373 Ma, indicating a variable lead loss up to 1.5%. The anomalously old 207Pb/235U and 207Pb/206Pb ages are consistent with the presence of excess radiogenic 207Pb* in the baddeleyite. We interpret this as a result of preferential partitioning of 231Pa to baddeleyite.Fifteen phlogopite and tetraferriphlogopite fractions from five carbonatite and phoscorite samples yielded precise Rb-Sr isochron age of 372.2 ± 1.5 Ma, which is 5 to 7 m.y. younger than our best estimate based on U-Th-Pb age values. This difference is unlikely to be a result of the disturbance or late closure of Rb-Sr system in phlogopite, but rather suggests that the accepted decay constant of 87Rb is too high.Comparative study of multiple geochronometer minerals from the Kovdor massif has revealed an exceptional complexity of isotopic systems. Reliable ages can be understood through systematic analysis of possible sources of distortion. No single geochronometer is sufficiently reliable in these rocks. Th-Pb and Rb-Sr can be a very useful supplement to U-Pb geochronometry, but the routine use of these geochronometers together will require more precise and accurate determination of decay constants for 232Th and 87Rb.  相似文献   

14.
Uranium (U) concentrations and activity ratios (δ234U) of authigenic carbonates are sensitive recorders of different fluid compositions at submarine seeps of hydrocarbon-rich fluids (“cold seeps”) at Hydrate Ridge, off the coast of Oregon, USA. The low U concentrations (mean: 1.3 ± 0.4 μg/g) and high δ234U values (165-317‰) of gas hydrate carbonates reflect the influence of sedimentary pore water indicating that these carbonates were formed under reducing conditions below or at the seafloor. Their 230Th/234U ages span a time interval from 0.8 to 6.4 ka and cluster around 1.2 and 4.7 ka. In contrast, chemoherm carbonates precipitate from marine bottom water marked by relatively high U concentrations (mean: 5.2 ± 0.8 μg/g) and a mean δ234U ratio of 166 ± 3‰. Their U isotopes reflect the δ234U ratios of the bottom water being enriched in 234U relative to normal seawater. Simple mass balance calculations based on U concentrations and their corresponding δ234U ratios reveal a contribution of about 11% of sedimentary pore water to the bottom water. From the U pore water flux and the reconstructed U pore water concentration a mean flow rate of about 147 ± 68 cm/a can be estimated. 230Th/234U ages of chemoherm carbonates range from 7.3 to 267.6 ka. 230Th/234U ages of two chemoherms (Alvin and SE-Knoll chemoherm) correspond to time intervals of low sealevel stands in marine isotope stages (MIS) 2, 4, 5, 6, 7 and 8. This observation indicates that fluid flow at cold seep sites sensitively reflects pressure changes of the hydraulic head in the sediments. The δ18OPDB ratios of the chemoherm carbonates support the hypothesis of precipitation during glacial times. Deviations of the chemoherm δ18O values from the marine δ18O record can be interpreted as to reflect temporally and spatially varying bottom water and/or vent fluid temperatures during carbonate precipitation between 2.6 and 8.6°C.  相似文献   

15.
Stilbite from Malmberget and Svappavara is part of hydrothermal mineral assemblages occupying regionally occurring open Palaeoproterozoic fractures in northern Sweden. At these locations, stilbite is characterized by Pbrad excess relative to U and by activity ratios of [234U]/[238U] > 1 and [230Th]/[238U] > 1. The activity disequilibrium requires a disturbance of the U-Th systematics within the last one million years. Leaching and infiltration experiments on Malmberget stilbite demonstrate: (i) preferential leaching in the order Pb >U >Th and uptake in the order Pb > U, and (ii) isotopic fractionation of U by preferential mobilization of 238U and 235U relative to 234U. Stepwise-leaching further indicates that the bulk of U is hosted in the channel sites of stilbite. The Th-U disequilibrium systematics observed in untreated Malmberget and Svappavara stilbite can be explained by: (1) addition of U with [234U]/[238U] > 1 from a fluid, or alternatively (2) loss of U from a two-component system, consisting of a component that is “open” or accessible and a component that is “closed” or inaccessible to mobilization. U addition requires a multistage history involving multiple gain or loss of U and/or Pb. In contrast, U loss does not necessarily require multistage processes but can also be explained by preferential removal of 238U (and 235U) relative to recoiled daughter isotopes such as 234U, 230Th, and 206Pb (and 207Pb) during a single event. Such a behavior could be obtained if the recoiled daughter isotopes of channel-sited uranium are implanted into the crystal lattice and, in such a way, become less mobile than their parent isotopes. This case implies an open-system behavior for ions in the channel sites and a closed-system behavior for ions in the silicate framework of stilbite. Each α-recoil directly or indirectly, i.e., through its recoil cascade, damages the silicate framework. Subsequent (continuous) low-temperature annealing of the damaged stilbite lattice could trap the recoiled daughter isotopes in the repaired crystal lattice or sealed-off channels. Such immobile recoiled material can, in part, represent the “closed” component of the system. This model can account for all observations regarding the Th-U-Pb systematics, including the Th-U disequilibrium systematics, the similarity in Th/U as deduced from Th-U disequilibrium and Pb isotope data, and the excess of radiogenic Pb (208Pb-parents also had been multiply recoiled). These two contrasting explanations involve either multistage or multicomponent systems. They do not permit the derivation of an accurate age.  相似文献   

16.
Interpretation of U-series disequilibria in midocean ridge basalts is highly dependent on the bulk partition coefficients for U and Th and therefore the mineralogy of the mantle source. Distinguishing between the effect of melting processes and variable source compositions on measured disequilibria (238U-230Th-226Ra and 235U-231Pa) requires measurement of the radiogenic isotopes Hf, Nd, Sr, and Pb. Here, we report measurements of 238U-230Th-226Ra and 235U-231Pa disequilibria; Hf, Nd, Sr, and Pb isotopic; and major and trace element compositions for a suite of 20 young midocean ridge basalts from the East Pacific Rise axis between 9°28′ and 9°52′N. All of the samples were collected within the axial summit trough using the submersible Alvin. The geological setting and observational data collected during sampling operations indicate that all the rocks are likely to have been erupted from 1991 to 1992 or within a few decades of that time. In these samples, 230Th excesses and 226Ra excesses are variable and inversely correlated. Because the eruption ages of the samples are much less than the half-life of 226Ra, this inverse correlation between 230Th and 226Ra excesses can be considered a primary feature of these lavas. For the lava suite analyzed in this study, 226Ra and 230Th excesses also vary with lava composition: 226Ra excesses are negatively correlated with Na8 and La/Yb and positively correlated with Mg#. Conversely, 230Th excesses are positively correlated with Na8 and La/Yb and negatively correlated with Mg#. Th/U, 230Th/232Th, and 230Th excesses are also variable and correlated to one another. 231Pa excesses are large but relatively constant and independent of Mg#, La/Yb, Th/U, and Na8. The isotope ratios 143Nd/144Nd, 176Hf/177Hf, 87Sr/86Sr, and 208Pb/206Pb are constant within analytical uncertainty, indicating that they were derived from a common source. The source is homogeneous with respect to parent/daughter ratios Lu/Hf, Sm/Nd, Rb/Sr, and Th/U; therefore, the measured variations of Th/U, 230Th, and 226Ra excesses and major and trace element compositions in these samples are best explained by polybaric melting of a homogeneous source, not by mixing of compositionally distinct sources.  相似文献   

17.
Extreme U and Pb isotope variations produced by disequilibrium in decay chains of 238U and 232Th are found in calcite, opal/chalcedony, and Mn-oxides occurring as secondary mineral coatings in the unsaturated zone at Yucca Mountain, Nevada. These very slowly growing minerals (mm my−1) contain excess 206Pb and 208Pb formed from excesses of intermediate daughter isotopes and cannot be used as reliable 206Pb/238U geochronometers. The presence of excess intermediate daughter isotopes does not appreciably affect 207Pb/235U ages of U-enriched opal/chalcedony, which are interpreted as mineral formation ages.Opal and calcite from outer (younger) portions of coatings have 230Th/U ages from 94.6 ± 3.7 to 361.3 ± 9.8 ka and initial 234U/238U activity ratios (AR) from 4.351 ± 0.070 to 7.02 ± 0.12, which indicate 234U enrichment from percolating water. Present-day 234U/238U AR is ∼1 in opal/chalcedony from older portions of the coatings. The 207Pb/235U ages of opal/chalcedony samples range from 0.1329 ± 0.0080 to 9.10 ± 0.21 Ma, increase with microstratigraphic depth, and define slow long-term average growth rates of about 1.2-2.0 mm my−1, in good agreement with previous results. Measured 234U/238U AR in Mn-oxides, which pre-date the oldest calcite and opal/chalcedony, range from 0.939 ± 0.006 to 2.091 ± 0.006 and are >1 in most samples. The range of 87Sr/86Sr ratios (0.71156-0.71280) in Mn-oxides overlaps that in the late calcite. These data indicate that Mn-oxides exchange U and Sr with percolating water and cannot be used as a reliable dating tool.In the U-poor calcite samples, measured 206Pb/207Pb ratios have a wide range, do not correlate with Ba concentration as would be expected if excess Ra was present, and reach a value of about 1400, the highest ever reported for natural Pb. Calcite intergrown with opal contains excesses of both 206Pb and 207Pb derived from Rn diffusion and from direct α-recoil from U-rich opal. Calcite from coatings devoid of opal/chalcedony contains 206Pb and 208Pb excesses, but no appreciable 207Pb excesses. Observed Pb isotope anomalies in calcite are explained by Rn-produced excess Pb. The Rn emanation may strongly affect 206Pb-238U ages of slow-growing U-poor calcite, but should be negligible for dating fast-growing U-enriched speleothem calcite.  相似文献   

18.
The Opalinus Clay formation in North Switzerland is a potential host rock for a deep underground radioactive waste repository. The distribution of 238U, 234U and 230Th was studied in rock samples of the Opalinus Clay from an exploratory borehole at Benken (Canton of Zurich) using MC-ICP-MS. The aim was to assess the in situ, long-term migration behaviour of 234U in this rock. Very low hydraulic conductivities of the Opalinus Clay, reducing potential of the pore water and its chemical equilibrium with the host rock are expected to render both 238U and 230Th immobile. If U is heterogeneously distributed in the Opalinus Clay, gradients in the supply of 234U from the rock matrix to the pore water by the decay of 238U will be established. Diffusive redistribution separates 234U from its immobile parent 238U resulting in bulk rock 234U/238U activity disequilibria. These may provide a means of estimating the mobility of 234U in the rock if the diffusion rate of 234U is significant compared to its decay rate. Sampling was carried out on two scales. Drilling of cm-spaced samples from the drill-core was done to study mobility over short distances and elucidate possible small-scale lithological control. Homogenized 25-cm-long portions of a 2-m-long drill-core section were prepared to provide information on transport over a longer distance. Variations in U and/or Th content on the cm-scale between clays and carbonate-sandy layers are revealed by β-scanning, which shows that the (dominant) clay is richer in both elements.  相似文献   

19.
U-Pb systems were examined in samples (ranging from 4 to 10 cm3 in volume) of ore material taken from along a 3.5-m profile across a zone of U mineralization exposed in an underground mine at the Strel’tsovskoe U deposit in eastern Transbaikalia. The behaviors of two isotopic U-Pb systems (238U-206Pb and 235U-207Pb) are principally different in all samples from our profile. While the individual samples are characterized by a vast scatter of their T(206Pb/238U) age values (from 112 to 717 Ma), the corresponding T(207Pb/235U) values vary much less significantly (from 127 to 142 Ma) and are generally close to the true age of the U mineralization. The main reason for the distortion of the U-Pb system is the long-lasting (for tens of million years) migration of intermediate decay products in the 238U-206Pb(RD238U) in the samples. This process resulted in the loss of RD238U from domains with high U concentrations and the subsequent accommodation of RD238U at sites with low U concentrations. The long-term effect of these opposite processes resulted in a deficit or excess of 206Pb as the final product of 238U decay. The loss or migration of RD238U are explained by the occurrence of pitchblende in association with U oxides that have higher Si and OH concentrations than those in the pitchblende and a higher +6U/+4U ratio. The finely dispersed character of the mineralization and the loose or metamict texture of the material are the principal prerequisites for RD238U loss and an excess of 206Pb in adjacent domains with low U concentrations. Domains with low U contents in the zone with U mineralization serve as geochemical barriers (because of sulfides contained in them) at which long-lived RD238U(226Ra, 210Po, 210Bi, and 210Pb) were accommodated and subsequently caused an excess of 206Pb. The 235U-207Pb system remained closed because of the much briefer lifetime of the 235U decay products. This may account for the significant discrepancies between the T(206Pb/238U) and T(207Pb/235U) age values. RD238U was most probably lost via the migration of radioisotopes at the middle part and end of the 238U family (starting with 226Ra). The heavy Th, Pa, and U radioisotopes (234Th, 234Pa, 234U, and 230Th) that occur closer to the beginning of 238U decay, before 226Ra, only relatively insignificantly participated in the process. Our results show that the loss and migration of RD238U are, under certain conditions, the main (or even the only) process responsible for the distortion of the U-Pb system.  相似文献   

20.
Reliable and precise ages of Quaternary pedogenic carbonate can be obtained with 230Th/U dating by thermal ionization mass spectrometry applied to carefully selected milligram-size samples. Datable carbonate can form within a few thousand years of surface stabilization allowing ages of Quaternary deposits and surfaces to be closely estimated. Pedogenic carbonate clast-rinds from gravels of glacio-fluvial terraces in the Wind River Basin have median concentrations of 14 ppm U and 0.07 ppm 232Th, with median (230Th/232Th) = 270, making them well suited for 230Th/U dating. Horizons as thin as 0.5 mm were sampled from polished slabs to reduce averaging of long (≥105 yr), and sometimes visibly discontinuous, depositional histories. Dense, translucent samples with finite 230Th/U ages preserve within-rind stratigraphic order in all cases. Ages for terraces WR4 (167,000 ± 6,400 yr) and WR2 (55,000 ± 8600 yr) indicate a mean incision rate of 0.26 ± 0.05 m per thousand years for the Wind River over the past glacial cycle, slower than inferred from cosmogenic-nuclide dating. Terrace WR3, which formed penecontemporaneously with the final maximum glacial advance of the penultimate Rocky Mountain (Bull Lake) glaciation, has an age of 150,000 ± 8300 yr indicating that it is broadly synchronous with the penultimate global ice volume maximum.  相似文献   

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