首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 39 毫秒
1.
Important He and Ar isotope studies on rocks and minerals, relevant to the geochemical and degassing history of the Earth, are often hampered by insufficient knowledge of the retentivity of different types of sites in minerals (inclusions, matrix) for these species, and of the relative importance of radiogenic and trapped components and possible differences in their behavior.To identify sites of noble gas isotopes, shed some light on their origin and estimate their residence times in olivine, which is a mineral considered as a good natural sampler, we investigated 2.5 Ga old ultramafic rocks from the Monche Pluton (Kola Peninsula, north-east part of the Baltic shield) using several extraction methods: crushing, fusion, slow step-wise and rapid incremental heating. Previous studies indicated that these rocks contain mainly trapped noble gases; however, to constrain the possible contribution of in-situ generated radiogenic helium, U and Th concentrations were also measured in the samples.The helium release pattern obtained by relatively fast (∼1.5 h long) incremental heating of olivine includes three distinct release peaks for helium: a low-temperature (600 °C) l-peak, a middle (800-1100 °C) m-peak and a high-temperature (∼1400 °C) h-peak. However, helium extraction from a powdered aliquot of the same olivine yields mainly the middle m-peak indicating that gases released in the l- and h-peaks occupy gas-liquid inclusions opened in the course of crushing and grinding. Moreover, slow step-wise heating (14 h) also results in a broad He release peak but in two well-separated l- and h-peaks of non-atmospheric 40Ar∗. This feature implies helium migration from l- and h-vesicles into the matrix m during long step-wise heating experiments, whereas less movable Ar remains in inclusions at even relatively high almost-magmatic temperatures.Using a simple phenomenological model envisaging the three different residence sites for noble gases, both fast- and slow-heating release patterns for 40Ar∗ and He, including those for the crushed sample, could be reproduced. The diffusion parameters inferred from the modeling of olivine (D0 = 2.4 × 10−2 cm2 s−1 and Ea = 133 kJ mol−1) are similar to those published by Shuster et al. (2003) and Blard et al. (2008). The high matrix/fluid solubility coefficient for helium, HHe ∼ 0.01, exceeds estimates reported by Trull and Kurz (1993); however, the product DHe(T) × HHe, the “permeability” (that governs He migration in vesicles + matrix composed materials), is very similar to their value. Extrapolation to the ambient temperature (0 °C) gives long and similar helium residence times in l- and h-vesicles, exceeding 1010 yrs, and even longer time scales ∼1016 yrs are obtained for the helium residence in the matrix. Therefore, at low temperatures our samples may be considered as excellent samplers of trapped volatile species, including helium.  相似文献   

2.
Recent work [Shuster D. L., Flowers R. M. and Farley K. A. (2006) The influence of natural radiation damage on helium diffusion kinetics in apatite. Earth Planet. Sci. Lett.249(3-4), 148-161] revealing a correlation between radiogenic 4He concentration and He diffusivity in natural apatites suggests that helium migration is retarded by radiation-induced damage to the crystal structure. If so, the He diffusion kinetics of an apatite is an evolving function of time and the effective uranium concentration in a cooling sample, a fact which must be considered when interpreting apatite (U-Th)/He ages. Here we report the results of experiments designed to investigate and quantify this phenomenon by determining He diffusivities in apatites after systematically adding or removing radiation damage.Radiation damage was added to a suite of synthetic and natural apatites by exposure to between 1 and 100 h of neutron irradiation in a nuclear reactor. The samples were then irradiated with a 220 MeV proton beam and the resulting spallogenic 3He used as a diffusant in step-heating diffusion experiments. In every sample, irradiation increased the activation energy (Ea) and the frequency factor (Do/a2) of diffusion and yielded a higher He closure temperature (Tc) than the starting material. For example, 100 h in the reactor caused the He closure temperature to increase by as much as 36 °C. For a given neutron fluence the magnitude of increase in closure temperature scales negatively with the initial closure temperature. This is consistent with a logarithmic response in which the neutron damage is additive to the initial damage present. In detail, the irradiations introduce correlated increases in Ea and ln(Do/a2) that lie on the same array as found in natural apatites. This strongly suggests that neutron-induced damage mimics the damage produced by U and Th decay in natural apatites.To investigate the potential consequences of annealing of radiation damage, samples of Durango apatite were heated in vacuum to temperatures up to 550 °C for between 1 and 350 h. After this treatment the samples were step-heated using the remaining natural 4He as the diffusant. At temperatures above 290 °C a systematic change in Tc was observed, with values becoming lower with increasing temperature and time. For example, reduction of Tc from the starting value of 71 to ∼52 °C occurred in 1 h at 375 °C or 10 h at 330 °C. The observed variations in Tc are strongly correlated with the fission track length reduction predicted from the initial holding time and temperature. Furthermore, like the neutron irradiated apatites, these samples plot on the same Ea − ln(Do/a2) array as natural samples, suggesting that damage annealing is simply undoing the consequences of damage accumulation in terms of He diffusivity.Taken together these data provide unequivocal evidence that at these levels, radiation damage acts to retard He diffusion in apatite, and that thermal annealing reverses the process. The data provide support for the previously described radiation damage trapping kinetic model of Shuster et al. (2006) and can be used to define a model which fully accommodates damage production and annealing.  相似文献   

3.
Helium diffusivity was measured in synthetic rare-earth-element orthophosphates with systematically varying properties to evaluate potential controls on He transport in minerals. In the zircon structure phosphates (in this study, the phosphates of Tb, Dy, Ho, Er, Tm, Yb, and Lu as well as synthetic xenotime, YPO4), He diffusion is strongly anisotropic. Transport apparently proceeds preferentially through channels aligned with the c-axis. The activation energy for diffusion is almost the same (122 ± 6 kJ/mol) in all members of this family, but there is a monotonic decrease in Do with atomic number from TbPO4 (∼105 cm2/s) to LuPO4 (∼10 cm2/s). The c-parallel channels become increasingly constricted in the same sequence, likely accounting for the systematically decreasing diffusivity. The He closure temperature (r = 1 cm, dT/dt = 10 °C/Myr) increases with atomic number from 44 °C for TbPO4 to 88 °C for LuPO4. Diffusion of radiogenic helium from natural zircon and xenotime is much slower than these synthetic analogs predict, suggesting that coupled substitution of REE and P for Zr and Si and/or radiation damage profoundly modify the energetics of interstitial He diffusion. In particular, α-recoil may play a key role by damaging the continuity and integrity of the channels.Monazite structure phosphates (here La, Ce, Pr, Nd, Sm, and Gd phosphate) are far more He retentive than those of the zircon structure. Activation energies increase smoothly with atomic number from LaPO4 (183 kJ/mol) to NdPO4 (224 kJ/mol) then decrease again to GdPO4 (198 kJ/mol). Do values mimic this pattern, spanning a range from ∼10−1 cm2/s (GdPO4) to 104 cm2/s (NdPO4). Nevertheless, He closure temperatures increase monotonically with atomic number, from 300 °C in LaPO4 to 410 °C in GdPO4. No evidence was obtained bearing on diffusion anisotropy, but the monazite structure lacks through-going channels so it is not expected. Diffusion parameters for radiogenic helium in natural monazite are similar to those obtained on the synthetic analogs.Ionic porosity is not the primary control on He diffusion in the orthophosphates. Within a given structure and with limited elemental substitution, ionic porosity and He closure temperature are negatively correlated, as predicted. However, differences between crystal structures are far more important than ion packing density: at comparable ionic porosity the monazite structure phosphates have He closure temperatures ∼300 °C higher than the xenotime structure phosphates. Modifications to the structures by radiation damage likely play a similarly significant role in controlling He diffusion.  相似文献   

4.
We assess the role of fracturing and seismicity on fluid-driven mass transport of helium using groundwaters from the eastern Morongo Basin (EMB), California, USA. The EMB, located ∼200 km east of Los Angeles, lies within a tectonically active region known as the Eastern California Shear Zone that exhibits both strike-slip and extensional deformation. Helium concentrations from 27 groundwaters range from 0.97 to 253.7 × 10−7 cm3 STP g−1H2O, with corresponding 3He/4He ratios falling between 1.0 and 0.26 RA (where RA is the 3He/4He ratio of air). All groundwaters had helium isotope ratios significantly higher than the crustal production value of ∼0.02 RA. Dissolved helium concentrations were resolved into components associated with solubility equilibration, air entrainment, in situ production within the aquifer, and extraneous fluxes (both crustal and mantle derived). All samples contained a mantle helium-3 (3Hem) flux in the range of 4.5 to 1351 × 10−14 cm3 STP 3He cm−2 yr−1 and a crustal flux (J0) between 0.03 and 300 × 10−7 cm3 STP 4He cm−2 yr−1. Groundwaters from the eastern part of the basin contained significantly higher 3Hem and deep crustal helium-4 (4Hedc) concentrations than other areas, suggesting a localized source for these components. 4Hedc and 3Hem are strongly correlated, and are associated with faults in the basin. A shallow thermal anomaly in a >3,000 m deep graben in the eastern basin suggests upflow of fluids through active faults associated with extensional tectonics. Regional tectonics appears to drive large scale crustal fluid transport, whereas episodic hydrofracturing provides an effective mechanism for mantle-crust volatile transport identified by variability in the magnitude of degassing fluxes (3Hem and J0) across the basin.  相似文献   

5.
The atmospheric 3He/4He ratio has been considered to be constant on a global scale, because the residence time of helium is significantly longer than the mixing time in the atmosphere. However, this ratio may be decreasing with time owing to the anthropogenic release of crustal helium from oil and natural gas wells, although this observation has been disputed. Here, we present the 3He/4He ratios of old air trapped in historical slags in Japan and of modern surface air samples collected at various sites around the world, measured with a newly developed analytical system. In air helium extracted from metallurgical slag found at refineries in operation between AD 1603 and 1907 in Japan, we determined a mean 3He/4He ratio of (5106 ± 108) × 10-5 RHESJ (where RHESJ is the 3He/4He ratio of the Helium Standard of Japan), which is consistent with the previously reported value of (5077 ± 59) × 10-5 RHESJ for historical slags in France and United Arab Emirates and about 4% higher than that of average modern air, (4901 ± 4) × 10-5 RHESJ. This result implies that the air 3He/4He ratio has decreased with time as expected by anthropogenic causes. Our modern surface air samples revealed that the 3He/4He ratio increases from north to south at a rate of (0.16 ± 0.08) × 10-5 RHESJ/degree of latitude, suggesting that the low 3He/4He ratio originates in high-latitude regions of the northern hemisphere, which is consistent with the fact that most fossil fuel is extracted and consumed in the northern hemisphere.  相似文献   

6.
To better understand the composition, characteristics of helium diffusion, and size distribution of interplanetary dust particles (IDPs) responsible for the long-term retention of extraterrestrial 3He, we carried out leaching, stepped heating, and sieving experiments on pelagic clays that varied in age from 0.5 Ma to ∼90 Myr. The leaching experiments suggest that the host phase(s) of 3He in geologically old sediments are neither organic matter nor refractory phases, such as diamond, graphite, Al2O3, and SiC, but are consistent with extraterrestrial silicates, Fe-Ni sulfides, and possibly magnetite. Stepped heating experiments demonstrate that the 3He release profiles from the magnetic and non-magnetic components of the pelagic clays are remarkably similar. Because helium diffusion is likely to be controlled by mineral chemistry and structure, the stepped heating results suggest a single carrier that may be magnetite, or more probably a phase associated with magnetite. Furthermore, the stepped outgassing experiments indicate that about 20% of the 3He will be lost through diffusion at seafloor temperatures after 50 Myrs, while sedimentary rocks exposed on the Earth’s surface for the same amount of time would lose up to 60%. The absolute magnitude of the 3He loss is, however, likely to depend upon the 3He concentration profile within the IDPs, which is not well known. Contrary to previous suggestions that micrometeorites in the size range of 50-100 μm in diameter are responsible for the extraterrestrial 3He in geologically old sediments [Stuart, F.M., Harrop, P.J., Knott, S., Turner, G., 1999. Laser extraction of helium isotopes from Antarctic micrometeorites: source of He and implications for the flux of extraterrestrial 3He flux to earth. Geochim. Cosmochim. Acta63, 2653-2665], our sieving experiment demonstrates that at most 20% of the 3He is carried by particles greater than 50 μm in diameter. The size-distribution of the 3He-bearing particles implies that extraterrestrial 3He in sediments record the IDP flux rather than the micrometeorite flux.  相似文献   

7.
Fourier transform infrared spectrometry (FTIR) analyses of olivines from peridotite xenoliths found in southern African kimberlites indicate 0 to 80 ppm H2O concentrations. OH absorbance profiles across olivine grains show homogeneous H contents from core to edge for most samples. In one sample the olivines are H-free, while another has olivines characterized by lower H contents at the grain edges compared to the cores, indicating H loss during transport of the xenolith to the surface. Flat or near-flat H profiles place severe constraints on the duration of H loss from olivine grains, with implications for kimberlite magma ascent rates. Diffusion equations were used to estimate times of H loss of about 4 h for the sample with heterogeneous olivine H contents. Resulting kimberlite ascent rates are calculated to be 5-37 m s−1 minimum, although these estimates are highly dependent on volatile contents and degassing behavior of the host kimberlite magma. Xenolithic olivines from alkali basalts generally have lower H contents and more pronounced H diffusion profiles than do those from kimberlites. This difference is likely caused by higher magma temperatures and lower ascent rates of alkali basalts compared to kimberlites.  相似文献   

8.
Hydrothermal treatment of closely sized muscovite aggregates in a piston-cylinder apparatus induced 40Ar loss that is revealed in 40Ar/39Ar step heating spectra. Age spectra and Arrhenius data, however, differ from that expected from a single diffusion length scale. A numerical model of episodic loss assuming the presence of multiple diffusion domains yields excellent fits between synthetic and actual degassing spectra. We used this model to isolate 40Ar loss from the grains that remained intact during hydrothermal treatment at 10 kbar permitting calculation of diffusion coefficients in the temperature range 730-600 °C. Diffusion data generated in this manner yield an activation energy (E) of 63 ± 7 kcal/mol and frequency factor (Do) of 2.3  cm2/s. Experiments at 20 kbar yield diffusivities lower by about an order of magnitude and correspond to an activation volume of ∼14 cm3/mol. Together, these parameters predict substantially greater retentivity of Ar in muscovite than previously assumed and correspond to a closure temperature (Tc) of 425 °C for a 100 μm radius grain cooling at 10 °C/Ma at 10 kbar (Tc = 405 °C at 5 kbar. Age and log (r/ro) spectra for the run products show strong correlations indicating that muscovites can retain Ar diffusion boundaries and mechanisms that define their natural retentivity during vacuum step heating. This may permit the application of high resolution, continuous 40Ar/39Ar thermochronology to low grade, regionally metamorphosed terranes.  相似文献   

9.
Laser depth profiling studies of helium diffusion in Durango fluorapatite   总被引:1,自引:0,他引:1  
Ultraviolet lasers coupled with sensitive mass spectrometers provide a useful way to measure laboratory-induced noble gas diffusion profiles in minerals, thus enabling the calculation of diffusion parameters. We illustrate this laser ablation depth profiling (LADP) technique for a previously well-studied mineral-isotopic system: 4He in Durango fluorapatite. LADP studies were conducted on oriented, polished slabs from a single crystal that were heated under vacuum to a variety of temperatures between 300 and 450 °C for variable times. The resolved 4He profiles exhibited error-function loss as predicted by previous bulk 4He diffusion studies. All of the slabs, regardless of crystallographic orientation, yielded modeled diffusivities that are statistically co-linear on an Arrhenius diagram, suggesting no diffusional anisotropy of 4He in this material. The data indicate an activation energy of 142.2 ± 5.0 (2σ) kJ/mol and diffusivity at infinite temperature - reported as ln(D0) - of −4.71 ± 0.94 (2σ) m2/s. These values imply a bulk closure temperature for 4He in Durango fluorapatite of 74 °C for a 50 μm radius grain, infinite cylinder geometry, and a cooling rate of 10 °C/Myr.  相似文献   

10.
A natural quartz sample free of mineral and fluid inclusions was irradiated with a 200 MeV proton beam to produce spallogenic 21Ne, 3He and 4He. Temperature-dependent diffusivities of these three nuclides were then determined simultaneously by high precision stepped-heating and noble gas mass spectrometry. The outward mobility of proton-induced nuclides reflects diffusion through the quartz lattice. In the studied range of 70 to 400°C the helium diffusion coefficients exceed those of neon by 5-7 orders of magnitude. The implied diffusion parameters Ea = 153.7 ± 1.5 (kJ/mol) and ln(Do/a2) = 15.9 ± 0.3 (ln(s−1)) and Ea = 84.5 ± 1.2 (kJ/mol) and ln(Do/a2) = 11.1 ± 0.3 (ln(s−1)) for proton-induced 21Ne and 3He, respectively, indicate that cosmogenic neon will be quantitatively retained in inclusion-free quartz at typical Earth surface temperatures whereas cosmogenic helium will not. However, the neon diffusion parameters also indicate that diffusive loss needs to be considered for small (<1 mm) quartz grains that have experienced elevated temperatures. Since natural quartz often contains fluid inclusions which may enhance noble gas retentivity, these parameters likely represent an end-member case of purely solid-state diffusion. The ∼70 kJ/mol higher activation energy for neon diffusion compared to helium diffusion likely represents an energy barrier related to its ∼13% greater diameter and provides a fundamental constraint with which to test theories of solid state diffusion. The diffusion parameters for proton-induced 4He are indistinguishable from those for 3He, providing no evidence for the commonly expected inverse square root of the mass diffusion relationship between isotopes. We also find preliminary indication that increased exposure to radiation may enhance neon and helium retentivity in quartz at low temperatures.  相似文献   

11.
In the last decade the zircon (U-Th)/He (ZHe) thermochronometer has been applied to a variety of geologic problems. Although bulk diffusion coefficients for He in zircon are available from laboratory step-heating experiments, little is known about the diffusion mechanism(s) and their dependence on the crystallographic structure of zircon. Here, we investigate the diffusion of He in perfectly crystalline zircon using atomistic simulation methods that provide insights into the structural pathways of He migration in zircon. Empirical force fields and quantum-mechanical calculations reveal that the energy barriers for He diffusion are strongly dependent on structure. The most favorable pathway for He diffusion is the [0 0 1] direction through the open channels parallel to the c-axis (, activation energy for tracer diffusion of a He atom along [0 0 1]). In contrast, energy barriers are higher in other directions where narrower channels for He diffusion are identified, such as [1 0 0], [1 0 1], and [1 1 0] (ΔE of 44.8, 101.7, and 421.3 kJ mol−1, respectively). Molecular dynamics simulations are in agreement with these results and provide additional insight in the diffusion mechanisms along different crystallographic directions, as well as the temperature dependence. Below the closure temperature of He in zircon [Tc ∼ 180 °C, Reiners P. W., Spell T. L., Nicolescu S., and Zanetti K. A. (2004) Zircon (U-Th)/He thermochronometry: He diffusion and comparisons with Ar-40/Ar-39 dating. Geochim. Cosmochim. Acta68, 1857-1887], diffusion is anisotropic as He moves preferentially along the [0 0 1] direction, and calculated tracer diffusivities along the two most favorable directions differ by approximately five orders of magnitude (D[001]/D[100] ∼ 105, at T = 25 °C). Above this temperature, He atoms start to hop between adjacent [0 0 1] channels, along [1 0 0] and [0 1 0] directions (perpendicular to the c-axis). The diffusion along [1 0 0] and [0 1 0] is thermally activated, such that at higher temperatures, He diffusion in zircon becomes nearly isotropic (D[001]/D[100] ∼ 10, at T = 580 °C). These results suggest that the anisotropic nature of He diffusion at temperatures near the closure temperature should be considered in future diffusivity experiments. Furthermore, care should be taken when making geologic interpretations (e.g., exhumation rates, timing of cooling, etc.) from this thermochronometer until the effects of anisotropic diffusion on bulk ages and closure temperature estimates are better quantified.  相似文献   

12.
We present new He-Ne data for geothermal fluids and He-Ne-Ar data for basalts from throughout the Icelandic neovolcanic zones and older parts of the Icelandic crust. Geothermal fluids, subglacial glasses, and mafic phenocrysts are characterized by a wide range in helium isotope ratios (3He/4He) encompassing typical MORB-like ratios through values as high as 36.8 RA (where RA = air 3He/4He). Although neon in geothermal fluids is dominated by an atmospheric component, samples from the northwest peninsula show a small excess of nucleogenic 21Ne, likely produced in-situ and released to circulating fluids. In contrast, geothermal fluids from the neovolcanic zones show evidence of a contribution of mantle-derived neon, as indicated by 20Ne enrichments up to 3% compared to air. The neon isotope composition of subglacial glasses reveals that mantle neon is derived from both depleted MORB-mantle and a primordial, ‘solar’ mantle component. However, binary mixing between these two endmembers can account for the He-Ne isotope characteristics of the basalts only if the 3He/22Ne ratio of the primordial mantle endmember is lower than in the MORB component. Indeed, the helium to neon elemental ratios (4He/21Ne∗ and 3He/22Nes where 21Ne∗ = nucleogenic 21Ne and 22Nes = ‘solar’-derived 22Ne) of the majority of Icelandic subglacial glasses are lower than theoretical values for Earth’s mantle, as observed previously for other OIB samples. Helium may be depleted relative to neon in high-3He/4He ratio parental melts due to either more compatible behavior during low-degree partial melting or more extensive diffusive loss relative to the heavier noble gases. However, Icelandic glasses show higher 4He/40Ar∗ (40Ar∗ = radiogenic Ar) values for a given 4He/21Ne∗ value compared to the majority of other OIB samples: this observation is consistent with extensive open-system equilibrium degassing, likely promoted by lower confining pressures during subglacial eruptions of Icelandic lavas. Taken together, the He-Ne-Ar systematics of Icelandic subglacial glasses are imprinted with the overlapping effects of helium depletion in the high-3He/4He ratio parental melt, binary mixing of two distinct mantle components, degassing fractionation and interaction with atmospheric noble gases. However, it is still possible to discern differences in the noble gas characteristics of the Icelandic mantle source beneath the neovolcanic zones, with MORB-like He-Ne isotope features prevalent in the Northern Rift Zone and a sharp transition to more primitive ‘solar-like’ characteristics in central and southern Iceland.  相似文献   

13.
《Applied Geochemistry》2001,16(4):419-436
The chemical and isotopic compositions of gases from hydrocarbon systems of the Taranaki Basin of New Zealand (both offshore and onshore) show wide variation. The most striking difference between the western and south-eastern groups of gases is the helium content and its isotopic ratio. In the west, the Maui gas is over an order of magnitude higher in helium concentration (up to 190 μmol mol−1) and its 3He/4He ratio of 3.8 RA (where RA=the air 3He/4He ratio of 1.4×10−6) is approximately half that of upper mantle helium issuing from volcanic vents of the Taupo Volcanic Zone. In the SE, the Kupe South and most Kapuni natural gases have only a minor mantle helium input of 0.03–0.32 RA and low total helium concentrations of 10–19 μmol mol−1. The 3He/C ratio (where C represents the total carbon in the gas phase) of the samples measured including those from a recent study of on-shore Taranaki natural gases are generally high at locations where the surface heat flow is high. The 3He/CO2 ratio of the Maui gases of 5 to 18×10−9 is higher than the MORB value of 0.2 to 0.5×10−9, a feature found in other continental basins such as the Pannonian and Vienna basins and in many high helium wells in the USA. Extrapolation to zero CO2/3He and CO2/C indicates δ13C(CO2) values between −7 and −5‰ close to that of MORB CO2. The remaining CO2 would appear to be mostly organically-influenced with δ13C(CO2) c.−15‰. There is some evidence of marine carbonate CO2 in the gases from the New Plymouth field. The radiogenic 4He content (Herad) varies across the Taranaki Basin with the highest Herad/C ratios occurring in the Maui field. δ13C(CH4) becomes more enriched in 13C with increasing Herad and hydrocarbon maturity. Because 3He/4He is related to the ratio of mantle to radiogenic crustal helium and 3He/C is virtually constant in the Maui field, there is a correlation between RC/RA (where RC=air-corrected 3He/4He) and δ13C(CH4) in the Maui and New Plymouth fields, with the more negative δ13C(CH4) values corresponding to high 3He/4He ratios. A correlation between 3He/4He and δ13C(CO2) was also observed in the Maui field. In the fields adjacent to Mt Taranaki (2518 m andesitic volcano), correlations of some parameters, particularly CO2/CH4, C2H6/CH4 and δ13C(CH4), are present with increasing depth of the gas reservoir and with distance from the volcanic cone.  相似文献   

14.
A correlation of petrography, mineral chemistry and in situ oxygen isotopic compositions of fine-grained olivine from the matrix and of fine- and coarse-grained olivine from accretionary rims around Ca-Al-rich inclusions (CAIs) and chondrules in CV chondrites is used here to constrain the processes that occurred in the solar nebula and on the CV parent asteroid. The accretionary rims around Leoville, Vigarano, and Allende CAIs exhibit a layered structure: the inner layer consists of coarse-grained, forsteritic and 16O-rich olivine (Fa1-40 and Δ17O = −24‰ to −5‰; the higher values are always found in the outer part of the layer and only in the most porous meteorites), whereas the middle and the outer layers contain finer-grained olivines that are more fayalitic and 16O-depleted (Fa15-50 and Δ17O = −18‰ to +1‰). The CV matrices and accretionary rims around chondrules have olivine grains of textures, chemical and isotopic compositions similar to those in the outer layers of accretionary rims around CAIs. There is a correlation between local sample porosity and olivine chemical and isotopic compositions: the more compact regions (the inner accretionary rim layer) have the most MgO- and 16O-rich compositions, whereas the more porous regions (outer rim layers around CAIs, accretionary rims around chondrules, and matrices) have the most MgO- and 16O-poor compositions. In addition, there is a negative correlation of olivine grain size with fayalite contents and Δ17O values. However, not all fine-grained olivines are FeO-rich and 16O-poor; some small (<1 μm in Leoville and 5-10 μm in Vigarano and Allende) ferrous (Fa>20) olivine grains in the outer layers of the CAI accretionary rims and in the matrix show significant enrichments in 16O (Δ17O = −20‰ to −10‰). We infer that the inner layer of the accretionary rims around CAIs and, at least, some olivine grains in the finer portions of accretionary rims and CV matrices formed in an 16O-rich gaseous reservoir, probably in the CAI-forming region. Grains in the outer layers of the CAI accretionary rims and in the rims around chondrules as well as matrix may have also originated as 16O-rich olivine. However, these olivines must have exchanged O isotopes to variable extents in the presence of an 16O-poor reservoir, possibly the nebular gas in the chondrule-forming region(s) and/or fluids in the parent body. The observed trend in isotopic compositions may arise from mixtures of 16O-rich forsterites with grain overgrowths or newly formed grains of 16O-poor fayalitic olivines formed during parent body metamorphism. However, the observed correlations of chemical and isotopic compositions of olivine with grain size and local porosity of the host meteorite suggest that olivine accreted as a single population of 16O-rich forsterite and subsequently exchanged Fe-Mg and O isotopes in situ in the presence of aqueous solutions (i.e., fluid-assisted thermal metamorphism).  相似文献   

15.
New He and C relative abundance, isotope and concentration results from nine geothermal locations situated along an 800-km transect of the North Anatolian Fault Zone (NAFZ), Turkey, that were monitored during the period November 2001–November 2004, are reported. The geothermal waters were collected every 3–6 months to study possible links between temporal geochemical variations and seismic activity along the NAFZ. At the nine sample locations, the He isotope ratios range from 0.24 to 2.3RA, δ13C values range from −4.5 to +5.8‰, and CO2/3He ratios range from 5 × 109 to 5 × 1014. The following geochemical observations are noted: (1) the highest 3He/4He ratios are found near the Galatean volcanic region, in the central section of the NAFZ, (2) at each of the nine sample locations, the 3He/4He ratios are generally constant; however, CO2/3He ratios and He contents both show one order of magnitude variability, and δ13C values show up to ∼4‰ variability, and (3) at all locations (except Re?adiye), δ13C values show positive correlations with CO2 contents. The results indicate that at least three processes are necessary to account for the geochemical variations: (1) binary mixing between crustal and mantle-derived volatiles can explain the general characteristics of 3He/4He ratios, δ13C values, and CO2/3He ratios at the nine sample locations; (2) preferential degassing of He from the geothermal waters is responsible for variations in CO2/3He values and He contents at each sample location; and (3) CO2 dissolution followed by calcite precipitation is responsible for variations in CO2 contents and δ13C values at most locations. For each of the geochemical parameters, anomalies are defined in the temporal record by values that fall outside two standard deviations of average values at each specific location. Geochemical anomalies that may be related to seismic activity are recorded on June 28, 2004 at Yalova, where a M = 4.2 earthquake occurred 43 days earlier at 15 km distance from the sample location, and on April 7, 2003 at Efteni, where a M = 4.0 earthquake occurred 44 days later at a distance of 12 km. At both locations, the sampling periods containing geochemical anomalies were preceded by an increase in M ? 3 earthquakes occurring within 60 days and less than 40 km distance.  相似文献   

16.
In the deep-sea, the Paleocene-Eocene Thermal Maximum (PETM) is often marked by clay-rich condensed intervals caused by dissolution of carbonate sediments, capped by a carbonate-rich interval. Constraining the duration of both the dissolution and subsequent cap-carbonate intervals is essential to computing marine carbon fluxes and thus testing hypotheses for the origin of this event. To this end, we provide new high-resolution helium isotope records spanning the Paleocene-Eocene boundary at ODP Site 1266 in the South Atlantic. The extraterrestrial 3He, 3HeET, concentrations replicate trends observed at ODP Site 690 by Farley and Eltgroth (2003). By assuming a constant flux of 3HeET we constrain relative changes in accumulation rates of sediment across the PETM and construct a new age model for the event. In this new chronology the zero carbonate layer represents 35 kyr, some of which reflects clay produced by dissolution of Paleocene (pre-PETM) sediments. Above this layer, carbonate concentrations increase for ∼165 kyr and remain higher than in the latest Paleocene until 234 +48/−34 kyr above the base of the clay. The new chronology indicates that minimum δ13C values persisted for a maximum of 134 +27/−19 kyr and the inflection point previously chosen to designate the end of the CIE recovery occurs at 217 +44/−31 kyr. This allocation of time differs from that of the cycle-based age model of Röhl et al. (2007) in that it assigns more time to the clay layer followed by a more gradual recovery of carbonate-rich sedimentation. The new model also suggests a longer sustained δ13C excursion followed by a more rapid recovery to pre-PETM δ13C values. These differences have important implications for constraining the source(s) of carbon and mechanisms for its subsequent sequestration, favoring models that include a sustained release of carbon after an initial pulse.  相似文献   

17.
Diffuse CO2 efflux near the Ukinrek Maars, two small volcanic craters that formed in 1977 in a remote part of the Alaska Peninsula, was investigated using accumulation chamber measurements. High CO2 efflux, in many places exceeding 1000 g m−2 d−1, was found in conspicuous zones of plant damage or kill that cover 30,000–50,000 m2 in area. Total diffuse CO2 emission was estimated at 21–44 t d−1. Gas vents 3-km away at The Gas Rocks produce 0.5 t d−1 of CO2 that probably derives from the Ukinrek Maars basalt based on similar δ13C values (∼−6‰), 3He/4He ratios (5.9–7.2 RA), and CO2/3He ratios (1–2 × 109) in the two areas. A lower 3He/4He ratio (2.7 RA) and much higher CO2/3He ratio (9 × 1010) in gas from the nearest arc-front volcanic center (Mount Peulik/Ugashik) provide a useful comparison. The large diffuse CO2 emission at Ukinrek has important implications for magmatic degassing, subsurface gas transport, and local toxicity hazards. Gas–water–rock interactions play a major role in the location, magnitude and chemistry of the emissions.  相似文献   

18.
The study reports the age evolution of groundwater as it flows from the recharge area through a regional alluvial aquifer system in North Gujarat-Cambay region in western India. Radiocarbon (14C), 4He and 4He / 222Rn dating methods have been employed. Sediments from a drill core in the Cambay Basin were also analysed for uranium (U) and thorium (Th) concentrations and the measured values have been used to estimate the 4He and 222Rn production rate for groundwater age calculations. Additionally, factors controlling the distribution of 222Rn, 4He and temperature anomalies in groundwater, vis-à-vis their relation to the tectonic framework and lithology of the study area, have also been examined.The multi-isotope study indicated a reasonable correspondence in groundwater age estimates by the three methods employed. The groundwater 14C ages increased, progressively, in the groundwater flow direction: from the foothills of Aravalli Mountains in the east, and reached a value of ∼35 ka towards the region of lowest elevation, linking Little Rann of Kachchh (LRK)-Nalsarovar (NS)-Gulf of Khambhat (GK) in the western part of the study area. In this region, groundwater ages obtained for free flowing thermal wells and springs employing 4He and 4He / 222Rn systematics are in the order of million years. Such anomalous ages are possibly due to enhanced mobilisation and migration of ‘excess helium’ from hydrothermal circulation vents along deep-seated faults. Excluding such anomalous cases and considering all uncertainties, presently estimated 4He and 4He / 222Rn groundwater ages are in reasonable agreement with 14C age estimates in the Cambay Basin for helium release factor (ΛHe) value of 0.4 ± 0.3. The 4He method also indicated west-southwards progression of groundwater ages up to ∼100 ka beyond the Cambay Basin.Large ‘excess helium’ concentrations are also seen to be generally associated with anomalous groundwater temperatures (> 35 °C) and found to overlie some of the basement faults in the study area, particularly along the east and the west flanks of the Cambay Basin. Groundwater 222Rn activities in most of the study area are 800 ± 400 dpm/l. But, a thermal spring at Tuwa on the east flank of the Cambay Basin, having granitic basement at shallow depth, recorded the highest 222Rn activity (∼63,000 dpm/l).  相似文献   

19.
Geotechnical characterisation is undertaken for 3 broad units comprising the bulk of the stratigraphy identified on White Island Volcano, Bay of Plenty, New Zealand, an active island stratovolcano. Field and laboratory measurements were used to describe rock mass characteristics for jointed lava flow units, and ring shear tests were undertaken to derive residual strength parameters for joint infilling materials within the lavas. Rock Mass Rating (RMR) and Geological Strength Index (GSI) values were calculated and converted to Mohr-Coulomb strength parameters using the Hoek-Brown criterion. Backanalysis of known landslide scarps was used to derive strength parameters for brecciated rock masses and hydrothermally altered rock masses. Andesite lava flows have high intact strength (σci = 184 ± 50 MN m− 2; γ = 24.7 ± 0.3 kN m− 3) and typically 3 wide, infilled joint sets, one parallel to flow direction and two steeply inclined, with spacings of 0.3-1.7 m. Joints are rough, with estimated friction angles for clean joints of ?j = 42-47°. Joint infill materials are clayey silts derived from weathering of wall rocks and primary volcanic sources; they have low plastic (54%) and liquid (84%) limits and residual strength values of cr = 0 kN m− 2 and ?r = 23.9 ± 3.1°. RMR values range from 70 to 73, giving calculated strength parameters of c′ = 1161-3391 kN m− 2 and ?′ = 50.5-62.3°. Backanalysis suggests brecciated rock masses have c′ = 0 kN m− 2 and ?′ = 35.4°, whereas GSI observations in the field suggest higher cohesion (c′ = 306-719 kN m− 2) and a range of friction angles bracketing the backanalysed result (?′ = 30.6-41.7°). Hydrothermally altered rock masses have c′ = 369 kN m− 2 and ?′ = 14.9°, indicating considerable loss of strength, especially frictional resistance, compared with the fresh lava units. Values measured at outcrop scale in this study are in keeping with other published values for similar volcanic edifices; backanalysed data suggest weaker rock mass properties than those determined at outcrop. This is interpreted as a scale issue, whereby rock mass characteristics of a large rock mass (crater wall scale) are weaker than those of small outcrops, due in part to the overestimation of friction angle from measurements on small exposures.  相似文献   

20.
The interaction of the lanthanides (Ln) with humic substances (HS) was investigated with a novel chemical speciation tool, Capillary Electrophoresis-Inductively Coupled Plasma Mass Spectrometry (CE-ICP-MS). By using an EDTA-ligand competition method, a bi-modal species distribution of LnEDTA and LnHS is attained, separated by CE, and detected online by sector field ICP-MS. We quantified the binding of all 14 rare earth elements (REEs), Sc and Y with Suwannee river fulvic acid, Leonardite coal humic acid, and Elliot soil humic acid under environmental conditions (pH 6-9, 0.001-0.1 mol L−1 NaNO3, 1-1000 nmol L−1 Ln, 10-20 mg L−1 HS). Conditional binding constants for REE-HS interaction (Kc) ranged from 8.9 < log Kc < 16.5 under all experimental conditions, and display a lanthanide contraction effect, ΔLKc: a gradual increase in Kc from La to Lu by 2-3 orders of magnitude as a function of decreasing ionic radius. HS polyelectrolyte effects cause Kc to increase with increasing pH and decreasing ionic strength. ΔLKc increases significantly with increasing pH, and likely with decreasing ionic strength. Based on a strong correlation between ΔLKc values and denticity for organic acids, we suggest that HS form a range of tri- to tetra-dentate complexes under environmental conditions. These results confirm HS to be a strong complexing agent for Ln, and show rigorous experimental evidence for potential REE fractionation by HS complexation.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号