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1.
Tracer diffusion coefficients of 153Gd and 152Eu in olivine tholeiite have been determined at temperatures between 1150 and 1440°C. The results are identical for both tracers within experimental error. Between 1440 and 1320°C the diffusion coefficients are given by D(Eu, Gd) = 0.058 exp(?40,600/ RT). Between 1320 and 1210°C, the diffusion coefficients are constant at D = (1.4 ± 0.4) × 10?7 cm2s?1 and between 1210 and 1150°C, the D values drop irregularly to 4 × 10?9 cm2s?1. The liquidus temperature (1270°C) lies within the region of constant D. Such anomalous behavior has not been encountered in previous studies of Ca, Sr, Ba and Co diffusion in basalt. To explain the constant D value near the liquidus, we speculate that the structure of the melt changes as a function of temperature in such a way that the normal temperature dependence of the diffusivity is compensated. For example, the rare earth ions may be displaced from their (high temperature) octahedral coordination sites to other sites where they are more readily dissociated and therefore become progressively more mobile. The behavior below 1210°C may be the result of relatively stable complexes or molecules in the melt or of the formation of a REE bearing crystalline phase that has so far escaped detection. Preliminary results for Eu diffusion in obsidian are D (Eu, 800°C) = 5 × 10?13 cm2 s?1 and D (Eu, 950°C) = 1.5 × 10?11 cm2 s?1. These data are consistent with an activation energy of 59 Kcal mole?1. These low diffusivities indicate that the partitioning of REE in crystallizing intermediate and acidic melts may be controlled by diffusion in the melt rather than equilibrium between the crystal surface and the bulk melt.The diffusion data are applied to partial melting in the mantle, in an attempt to explain how LREE enriched tholeiites may be derived from a LREE depleted mantle source. In this model LREE diffuse from garnet bearing regions that have small melt fractions into garnet free regions that have relatively large melt fractions. REE diffusion is so slow that this process is quantitatively significant only in small partially molten bodies (diameter ～1 km or less) or in larger, but strongly flattened bodies. Internal convective motion during diapiric rise would also increase the efficiency of the process.  相似文献   

2.
《Applied Geochemistry》1998,13(6):707-714
The properties of fluorapatite, both a useful radiochronometer and a potential storage matrix specific for minor actinides produced by the reprocessing of spent nuclear fuel, have been investigated with emphasis to its response to alpha decay. Exfoliation, which occurs after implantation of high doses of 1.6-MeV He-ions (>1.4×1017 ions cm−2, corresponding to 5% atomic proportion), could set an upper limit to the concentration of imbedded actinides (about 2 atoms % corresponding to 20 wt. %) or storage age unless significant diffusion of radiogenic He intervenes. This process has been studied by combining He implantation, thermal treatments in the temperature range 124–250°C and measurement of the resulting He profile by an ion beam technique (ERDA) using 8.5-MeV C ions. The diffusion coefficient follows an Arrhenius' law with an activation energy of 120 (±2) KJ/mole and a frequency factor of 14.5 (±7)×10−3 cm2 sec−1 in agreement with literature data. The inferred closure temperature which validates the U,Th–He radiochronological method also fits previous values: 97 (±10)°C for grain size 165 μm. With respect to radwaste disposal. He volume diffusion is too small to exclude the occurrence of exfoliation unless diffusion at grain boundary is much higher and a fine-grain matrix is deliberately chosen.  相似文献   

3.
A workflow is described to estimate specific storage (S s) and hydraulic conductivity (K) from a profile of vibrating wire piezometers embedded into a regional aquitard in Australia. The loading efficiency, compressibility and S s were estimated from pore pressure response to atmospheric pressure changes, and K was estimated from the earliest part of the measurement record following grouting. Results indicate that S s and K were, respectively, 8.8?×?10?6 to 1.2?×?10?5 m?1 and 2?×?10?12 m s?1 for a claystone/siltstone, and 4.3?×?10?6 to 9.6?×?10?6 m?1 and 1?×?10?12 to 5?×?10?12 m s?1 for a thick mudstone. K estimates from the pore pressure response are within one order of magnitude when compared to direct measurement in a laboratory and inverse modelled flux rates determined from natural tracer profiles. Further analysis of the evolution and longevity of the properties of borehole grout (e.g. thermal and chemical effects) may help refine the estimation of formation hydraulic properties using this workflow. However, the convergence of K values illustrates the benefit of multiple lines of evidence to support aquitard characterization. An additional benefit of in situ pore pressure measurement is the generation of long-term data to constrain groundwater flow models, which provides a link between laboratory scale data and the formation scale.  相似文献   

4.
In order to test the chronometer qualities of speculante for the (U + Th)/He dating method, 4He release experiments by stepwise heating of two specularites from the Rimbach mineralization locality in the southern Vosgues (France) have been carried out. The diffusion coefficients define linear Arrhenius plots within a temperature interval of 250 to 830 °C, which is suggestive of volume diffusion. Extrapolation of the diffusion behavior to 20° C yields diffusion coefficients (D20 values) smaller than 10?26 [cm2 s?1] for both hematites with activation energies at 116 [kJ/mole]. The results of our study suggest that specularite is a very helium retentive hematite variety which is capable of quantitatively retaining radiogenic helium over geologic periods of time.  相似文献   

5.
Interdiffusion coefficients of Al + Al vs. Mg + Si in the gehlenite–åkermanite system of melilite were determined by coupled annealing of synthesized end-member single crystals. The observed diffusion coefficients for a couple-annealed sample vary for about 2 orders of magnitude, showing strong dependence on the gehlenite–åkermanite composition: diffusion coefficient observed at 1350 °C, for example, is 3 × 10?13 cm2 s?1 at 5 mol% åkermanite composition (Ak5), increases to 2 × 10?11 cm2 s?1 at Ak80, and then decreases to 1 × 10?12 cm2 s?1 at Ak95. The diffusion coefficient–temperature relation indicates high activation energy of diffusion of about 420 kJ mol?1 for gehlenite-rich melilite. The observed diffusion coefficient–composition relation may be explained by a combination of (1) the diffusion coefficient–melting temperature relation (Flynn's rule) and (2) the feasibility of local charge compensation, which can possibly be maintained more easily in the intermediate chemical composition. The high activation energy value for gehlenitic melilite appears to correspond to the complex diffusion mechanism. The observed highly variable diffusion coefficients suggest that gehlenite–åkermanite zoning in the melilite crystals in Ca, Al-rich inclusions in the carbonaceous meteorites may provide a sensitive indicator for the thermal history of the inclusions.  相似文献   

6.
The dissolution of chrysotile is studied in regard to the surfaces analysis by photoelectron spectrometry. After leaching of chrysotile (Provenance: Thetford; about 200 mg of fibers of 1 cm length) in nonstirred 0.1 N oxalic conditions, the composition of the mineral surfaces is determined by XPS; kinetic curves of dissolution are given in the range 22–80°C. Two conditions for the rate-limiting step are involved for the explanation of the dissolution: diffusion of Mg2+ through the fibrous gel or dissociation of chrysotile. By the former, some values of the diffusion coefficient are proposed: D varies from 5·10?19 cm2s?1 to 5·10?16 cm2s?1, in the range 22–80°C. By the second model, the leaching rate is estimated from 3 Å (22°C) per h to 250 Å (80°C) per h. For the 2 models, the activation heat energy is in the range 15–20 Kcal.  相似文献   

7.
Electron transport properties of single crystal and polycrystalline natural mineral galena (PbS) samples from the Trep?a mine, Yugoslavia, were determined using the photoacoustic frequency transmission technique. Their thermal diffusivity (D T≈0.16 × 10?5 m2 s?1), the coefficient of diffusion (D between 0.15×10?2 0.16×10?2 m2 s?1) and lifetime of the excess carrier (τ≈35 μs and the front and rear recombination velocity (s g≈65.5 m s?1 and s b≈66.4 m s?1, respectively), were calculated by comparing the experimental results and the theoretical photoacoustic amplitude and phase signals. The lattice parameter obtained by X-ray work was a?=5.936?Å. The free carrier concentration of these single-crystal samples was measured using the Hall method (N?=?3×1018 cm?3). Measurements of the optical reflectivity of the same samples, as a function of wavelength, in the infrared and far infrared ranges, were performed. In the far infrared range a free electron plasma frequency was observed and numerically analyzed, using the least-squares fitting procedure. The values of optical parameters were calculated and the value of the free carrier concentration obtained by the Hall method was confirmed.  相似文献   

8.
Ground waters in a Precambrian granitic batholith at the Whiteshell Nuclear Research Establishment (WNRE) in Pinawa, Manitoba contain between 5 × 10?5 and 10?1 cc STP/gH2O of radiogenic helium-4 but have relatively uniform 3He/4He ratios of between 0.6 × 10?8 and 2.3 × 103. The highest helium samples also contain radiogenic 21,22Ne produced by (α,n) or (n,α) reactions with other isotopes. As much as 1.8 × 10?9ccSTP/gH2O of excess 21Ne and 3.8 × 10?9ccSTP/gH2O of excess 22Ne have been measured. Helium and 21Ne ages of these ground waters, calculated on the basis of known crustal production rates of 4He and 21Ne, are unreasonably high (up to 2 × 105 years) and incompatible with the 14C ages and other isotopic and hydrogeologic data. Uranium enrichment in the flow porosity of the granite may dominate 4He and 21,22Ne production in this granite and mask the contributions from more typical U and Th concentrations in the rock matrix.At the Chalk River Nuclear Laboratories in Ontario helium concentrations in ground waters in a Precambrian monzonitic gneiss range from 1.5 × 10?7 to 8.7 × 10?4ccSTP/gH2O with the 3He/4He ratios ranging from 2.0 × 10?3 to 1.5 × 10?7. The highest helium concentrations may be attributable to the presence of a thick uraniferous pegmatite vein and yield helium ages more than two orders of magnitude higher than the 14C ages. Application of He age dating equations to ground waters from Precambrian granitic rocks requires knowledge of the nature of uranium and thorium enrichment in the subsurface in order to select appropriate values for porosity and uranium and thorium concentration in the rock.  相似文献   

9.
The kinetics of zoned garnet porphyroblast growth is exemplified in a sample of garnet-staurolite-biotite schist from the northern Ladoga region. The diffusion-controlled porphyroblast growth was accompanied by a decrease in the kinetic coefficient during phase reactions. Even at insignificant (1–2°C) thermal overstepping, the leading role of diffusion as a factor that controls kinetics of porphyroblast growth in medium-grade metapelites is consistent with the parameters of metamorphic crystallization: T = 500–650°C, t = 1 Ma; D A1 app = 10?14 cm2/s, L = 0.2–0.6 cm, r = 1–3 mm, ΔC Al = 1.5 × 10?4–1.5 × 10?3 mol/cm3.  相似文献   

10.
Helium‐3 is a stable cosmogenic isotope that can be used to determine the time interval during which a rock sample has been at or close to the Earth’s surface. As a result of the high production rate of ‘cosmogenic’3He (≈ 130 at g?1 year?1) and the low detection limit of modern mass spectrometers, it is possible to date exceptionally young surfaces (≈ 1000 years). The precision and accuracy of cosmogenic 3He measurements depend critically on the passive helium blank (produced by the metalwork of the extraction furnace) which can be significant relative to the sample signals. We have developed and constructed, at the CRPG (Nancy, France), a new high temperature furnace (< 1500 °C) to extract helium in minerals such as apatite, pyroxene and olivine at 1050, 1350 and 1450 °C, respectively. The furnace demonstrated an excellent helium extraction yield (> 99% for olivine and pyroxene for heating times of 20–30 min and temperatures in the range 1050–1450 °C) and low residual helium contributions (the blank, obtained under the same analytical conditions as for sample extraction: 1 × 10?15 mole 4He and < 4 × 10?21 mole 3He). This is approximately an order of magnitude lower than those reported by other laboratories using conventional furnaces.  相似文献   

11.
The weathering rates and mechanisms of three types of glassy rocks were investigated experimentally at 25 °C, pH 1.0 to 6.2, and reaction times as much as to 3 months. Changes in major element chemistry were monitored concurrently as a function of time in the aqueous solution and within the near surface region of the glass. Leach profiles, obtained by a HF leaching technique, displayed near-surface zones depleted in major cations. These zones increased in depth with increasing time and decreasing pH of reactions. Release rates into the aqueous solution were parabolic for Na and K and linear for Si and Al. A coupled weathering model, involving surface dissolution with concurrent diffusion of Na, K, and Al, produced a mass balance between the aqueous and glass phases. Steady state conditions are reached at pH 1.0 after approximately 3 weeks of reaction. Steady-state is not reached even after 3 months at pH 6.2.An interdiffusion model describes observed changes in Na diffusion profiles for perlite at pH 1.0. The calculated Na self-diffusion coefficient of 5 × 10?19 cm2·s?1 at 25°C approximates coefficients extrapolated from previously reported high temperature data for obsidian. The self-diffusion coefficient for H3O+, 1.2 × 10?20 cm2·s?1, is similar to measured rates of water diffusion during hydration of obsidian to form perlite.  相似文献   

12.
The validity of the thermodynamic cBΩ model is tested in terms of the experimentally determined diffusion coefficients of He in a natural Fe-bearing olivine (Fo90) and a synthetic end-member forsterite (Mg2SiO4) over a broad temperature range (250–950 °C), as reported recently by Cherniak and Watson (Geochem Cosmochim Acta 84:269–279, 2012). The calculated activation enthalpies for each of the three crystallographic axes were found to be (134 ± 5), (137 ± 13) and (158 ± 4) kJ mol?1 for the [100], [010] and [001] directions in forsterite, and (141 ± 9) kJ mol?1 for the [010] direction in olivine, exhibiting a deviation of <1 % with the corresponding reported experimental values. Additional point defect parameters such as activation volume, activation entropy and activation Gibbs free energy were calculated as a function of temperature. The estimated activation volumes (3.2–3.9 ± 0.3 cm3 mol?1) of He diffusion in olivine are comparable with other reported results for hydrogen and tracer diffusion of Mg cations in olivine. The pressure dependence of He diffusion coefficients was also determined, based on single experimental diffusion measurements at 2.6 and 2.7 GPa along the [001] direction in forsterite at 400 and 650 °C.  相似文献   

13.
Solubilities of noble gases in magnetite were determined by growing magnetite in a noble-gas atmosphere between 450 and 700°K. Henry's law is obeyed at pressures up to 10?2 atm for He, Ne, Ar and up to 10?5 atm for Kr, Xe, with the following distribution coefficients at 500° (cc STP g?1 atm?5): He 0.042, Ne 0.016, Ar 3.6, Kr 1.3, Xe 0.88, some 102–105 times higher than previous determinations on silicate and fluoride melts. Apparent heats of solution in kcal/mole are: He ?2.42 ±0.12, Ne ?2.20 ±0.10, Ar ?15.25 ±0.25, Kr ?13.0 ±0.3, Xe ?12-5 ± 0.5. These values, too, stand in sharp contrast with earlier determinations on melts which were small and positive, but are comparable to the values for clathrates. Presumably the gases are held in anion vacancies.Extrapolation of the magnetite data to the formation temperature of C1 chondrites, 360°K, shows that the Arp36 content of Orgueil magnetite could be acquired by equilibrium solubility at a total nebular pressure of 4 × 10?6 atm. In the absence of data for silicates (the principal host phase of planetary gas), an attempt is made to estimate the solubilities required to account for planetary gases in meteorites. These values do not appear grossly unreasonable in the light of the magnetite data, when structural differences between the two minerals are taken into account. It seems that equilibrium solubility may be able to account for four features of planetary gas: elemental ratios, amounts, correlations with other volatiles and retentive siting. It cannot account for the isotopic fractionation of planetary gas, however.  相似文献   

14.
The infinite dilution diffusion coefficient for Al(OH)4? necessary to calculate fluxes of dissolved Al between sediments and overlying waters, was determined at 25°C. Measurements were made using the diaphragm-cell method by diffusing Al(OH)4? spiked KBr solutions against KCL over a range of ionic strengths. The mean of 9 separate measurements gives 1.04 ± .02 × 10?5cm2/s as the infinite dilution diffusion coefficient for Al(OH)4? at 25°C.  相似文献   

15.
Measurements of the flux of very-high-energy (>1 TeV) gamma rays from the blazar 3C 66A obtained over four years are presented. The mean flux over the four-year period was (2.8±0.4)×10?11 cm?2 s?1. There is a correlation between the season-averaged flux of very-high-energy gamma rays and the observed optical radiation.  相似文献   

16.
About possibility of isotope dating of native gold by the (U-Th)/He method   总被引：2，自引：0，他引：2  
For investigation of helium in native gold, a new measuring complex was created and used: the high sensitivity mass spectrometer MSU-G (ZAO SKB “SPECTRON”). The sensitivity of measuring 4He was 5.3 × 10?13 cm3/g per impulse. Experiments in stepwise heating of samples have been carried out, and the kinetics of radiogenic 4He emanation from native gold was investigated. Migration parameters (activation energy and frequency factor) were determined. Model calculations of stability (closure temperature) of radiogenic 4He in the native gold structure with a given time and temperature of thermal influences were made using the data received. The concentration of 4He in native gold from the original deposit Nesterovskoe is (4.7 ± 0.1) × 10?5 cm3/g in the sample from the placer; from Chudnoe deposit, it is (3.8 ± 0.1) × 10?5 cm3/g; from sulfide deposits of Kitoiskii knot of Eastern Sayani, it is (1.9 ± 0.1) × 10?5 cm3/g; and from the South Muiskii ore region it is (8.7 ± 0.5) × 10?7 cm3/g. The received curve lines of kinetics of 4He emanation from native gold show that radiogenic helium is well bonded in the native gold structure: in all the examined samples, most 4He emanates only by reaching the temperature of 950–1000°C. A specific feature of the kinetics of radiogenic 4He emanation in all examined samples is an outburstlike emanation in the form of a peak of large amplitude in the area of temperatures near the melting temperature point of gold. This is stipulated by the existence of helium bubbles released by metals only while they melt. The spectrum of helium thermal desorption from native gold has a complicated form and is a result of superposition of several peaks. This proves the migration of groups of atoms located in the gold structure in different energy states. Very large values of the activation energy of helium migration from native gold were received: up to 161–176 kcal/mol. Extremely large values of the frequency factor, from 2 × 1018 to 3 × 1032, correspond to such values of activation energies. This is caused probably by helium migration in the form of gas bubbles. The received data indicate the very high stability of the (U-Th)/He isotope system in native gold. Using the (U-Th)/He method of isotope geochronology seems to be very promising for isotope dating of these strategic raw materials.  相似文献   

17.
The dehydration kinetics of serpentine was investigated using in situ high-temperature infrared microspectroscopy. The analyzed antigorite samples at room temperature show relatively sharp bands at around 3,655–3,660 cm?1 (band 1), 3,570–3,595 cm?1 (band 2), and 3,450–3,510 cm?1 (band 3). Band 1 corresponds to the Mg–OH bond, and bands 2 and 3 correspond to OH associated with the substitution of Al for Si. Isothermal kinetic heating experiments at temperatures ranging from 625 to 700 °C showed a systematic decrease of the OH band absorbance with heating duration. The one-dimensional diffusion was found to provide the best fit to the experimental data, and diffusion coefficients were determined with activation energies of 219 ± 37 kJ mol?1 for the total water band area, 245 ± 46 kJ mol?1 for band 1, 243 ± 57 kJ mol?1 for band 2, and 256 ± 53 kJ mol?1 for band 3. The results indicate that the dehydration process is controlled by one-dimensional diffusion through the tetrahedral geometry of serpentine. Fluid production rates during antigorite dehydration were calculated from kinetic data and range from 3 × 10?4 to 3 × 10?5  $ {\text{m}}_{\text{fluid}}^{ 3} \,{\text{m}}_{\text{rock}}^{ - 3} \,{\text{s}}^{ - 1} $ . The rates are high enough to provoke hydraulic rupture, since the relaxation rates of rocks are much lower than these values. The results suggest that the rapid dehydration of antigorite can trigger an intermediate-depth earthquake associated with a subducting slab.  相似文献   

18.
Sized aggregates of glasses (47–84 wt% SiO2) were fused from igneous-derived cohesive fault rock and igneous rock, and step-heated from ~400 to >1,200 °C to obtain their 39Ar diffusion properties (average E=33,400 cal mol?1; D o=4.63×10?3 cm2 s?1). At T<~1,000 °C, glasses containing <~69 wt% SiO2 and abundant network-forming cations (Ca, Fe, Mg) reveal moderate to strong non-linear increases in D and E, reflecting structural modifications as the solid transitions to melt. Extrapolation of these Arrhenius properties down to typical geologic T-t conditions could result in a 1.5 log10 unit underestimation in the diffusion rate of Ar in similar materials. Numerical simulations based upon the diffusion results caution that some common geologic glasses will likely yield 40Ar/39Ar cooling ages rather than formation ages. However, if cooling rates are sufficiently high, ambient temperatures are sufficiently low (e.g., <65–175 °C), and coarse particles (e.g., radius (r) >~1 mm) are analyzed, glasses with compositions similar to ours may preserve their formation ages.  相似文献   

19.
We have investigated the effect of undercooling and deformation on the evolution of the texture and the crystallization kinetics of remelted basaltic material from Stromboli (pumice from the March 15, 2007 paroxysmal eruption) and Etna (1992 lava flow). Isothermal crystallization experiments were conducted at different degrees of undercooling and different applied strain rate (T = 1,157–1,187 °C and $ \dot{\gamma }_{i} $ γ · i  = 4.26 s?1 for Stromboli; T = 1,131–1,182 °C and $ \dot{\gamma }_{i} $ γ · i  = 0.53 s?1 for Etna). Melt viscosity increased due to the decrease in temperature and the increase in crystal content. The mineralogical assemblage comprises Sp + Plg (dominant) ± Cpx with an overall crystal fraction (?) between 0.06 and 0.27, increasing with undercooling and flow conditions. Both degree of undercooling and deformation rate deeply affect the kinetics of the crystallization process. Plagioclase nucleation incubation time strongly decreases with increasing ΔT and flow, while slow diffusion-limited growth characterizes low ΔT—low deformation rate experiments. Both Stromboli (high strain rate) and Etna (low strain rate) plagioclase growth rates (G) display relative small variations with Stromboli showing higher values (4.8 ± 1.9 × 10?9 m s?1) compared to Etna (2.1 ± 1.6 × 10?9 m s?1). Plagioclase average nucleation rates J continuously increase with undercooling from 1.4 × 106 to 6.7 × 106 m?3 s?1 for Stromboli and from 3.6 × 104 to 4.0 × 106 m?3 s?1 for Etna. The extremely low value of 3.6 × 104 m?3 s?1 recorded at the lowest undercooling experiment for Etna (ΔT = 20 °C) indicates that the crystallization process is growth-dominated and that possible effects of textural coarsening occur. G values obtained in this paper are generally one or two orders of magnitude higher compared to those obtained in the literature for equivalent undercooling conditions. Stirring of the melt, simulating magma flow or convective conditions, facilitates nucleation and growth of crystals via mechanical transportation of matter, resulting in the higher J and G observed. Any modeling pertaining to magma dynamics in the conduit (e.g., ascent rate) and lava flow emplacement (e.g., flow rate, pāhoehoe–‘a‘ā transition) should therefore take the effects of dynamic crystallization into account.  相似文献   

20.
Cobalt and magnesium interdiffusion coefficients in synthetic crystals of olivine have been determined by a method of couple annealing. These coefficients increase with temperature and Co concentration. The coefficients in forsterite along the c crystallographic axis range from 1.13 × 10?12 to 6.85 × 10?11 cm2sec?1 at temperatures ranging from 1150 to 1400°C. The calculated activation energies for Co-Mg interdiffusion in forsterite are 526 kJmol?1 above approximately 1300°C and 196 kJmol?1 at lower temperatures. These results indicate that the Co-Mg mobility in olivine is relatively low compared to published results for Fe-Mg interdiffusion.  相似文献   

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