Exfoliation and diffusion following helium ion implantation in fluorapatite: implications for radiochronology and radioactive waste disposal

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.     

He,Pb, Sr and Nd isotope constraints on magma genesis and mantle heterogeneity beneath young Pacific seamounts

Pb, Sr and Nd isotope variations are correlated in diverse lavas erupted at small seamounts near the East Pacific Rise. Tholeiites are isotopically indistinguishable from MORB (²⁰⁶Pb/²⁰⁴Pb=18.1–18.5; ⁸⁷Sr/⁸⁶Sr=0.7023–0.7028; ¹⁴³Nd/¹⁴⁴Nd=0.51326-0.51308); associated alkali basalts always show more radiogenic Pb and Sr signatures (²⁰⁶Pb/²⁰⁴Pb=18.8–19.2; ⁸⁷Sr/⁸⁶Sr=0.7029–0.7031) and less radiogenic Nd (¹⁴³Nd/¹⁴⁴Nd=0.51289–0.51301). The isotopic variability covers 80% of the variability for Pacific MORB, due to the presence of small-scale heterogeneity in the underlying mantle. Isotope compositions also correlate with trace element ratios such as La/Sm. Tholeiites at these seamounts have ³He/⁴He between 7.8–8.7 R _A(R _A= atmospheric ratio), also indistinguishable from MORB. He trapped in vesicles of alkali basalts, released by crushing in vacuo, has low ³He/⁴He (1.2–2.6 R)_Ain conjunction with low helium concentrations ([He]<5×10^–8 ccSTP/g). In many cases post-eruptive radiogenic ingrowth has produced He isotope disequilibrium between vesicles and glass in the alkali basalts; subatmospheric ³He/⁴He ratios characterize the He dissolved in the glass which is released by melting the crushed powders. The narrow range of ³He/⁴He in the vesicles of the alkali basalts suggests that low ³He/⁴He is a source characteristic, but given their low [He] and high (U + Th), pre-eruptive radiogenic ingrowth cannot be excluded as a cause for low inherited ³He/⁴He ratios. Pb, Sr and Nd isotope compositions in lavas erupted at Shimada Seamount, an isolated volcano on 20 m.y. old seafloor at 17°N, are distinctly different from other seamounts in the East Pacific (²⁰⁶Pb/²⁰⁴Pb=18.8–19.0, ⁸⁷Sr/ ⁸⁶Sr0.7048 and ¹⁴³Nd/¹⁴⁴Nd0.51266). Relatively high ²⁰⁷Pb/²⁰⁴Pb (15.6–15.7) indicates ancient (>2 Ga) isolation of the source from the depleted upper mantle, similar to Dupal components which are more prevalent in the southern hemisphere mantle. ³He/⁴He at Shimada Seamount is between 3.9–4.8 R _A. Because the helium concentrations range up to 1.5×10^–6, the low ³He/⁴He can not be due to radiogenic accumulation of ⁴He in the magma for reasonable volcanic evolution times. The low ³He/⁴He may be due to the presence of enriched domains within the lithosphere with high (U + Th)/He ratios, possibly formed during its accretion near the ridge. Alternatively, the low ³He/⁴He may be an inherent characteristic of an enriched component in the mantle beneath the East Pacific. Collectively, the He-Pb-Sr-Nd isotope systematics at East Pacific seamounts suggest that the range of isotope compositions present in the mantle is more readily sampled by seamount and island volcanism than by axial volcanism. Beneath thicker lithosphere away from the ridge axis, smaller degrees of melting in the source regions are less efficient in averaging the chemical characteristics of small-scale heterogeneities.     

The decay products of 222rn in etched track radon detection

Precipitation of decay products of atmospheric ²²²Rn in small containers and the effects of their precipitation on alpha-particle-track-measurements of radon activities were studied. From decay curves of decay product activities on surfaces exposed to radon-containing air the ratios ²¹⁴Pb/²¹⁸Po (=r) in the precipitates were determined. From r average ages of precipitating decay products were calculated. Average ages and r were low, indicating rapid precipitation of decay products, and decreased with container size. Activities on exposed surfaces were approximately those expected if decay products precipitate completely and uniformly on the internal surfaces of containers.Decay products precipitated on foils of correct thickness covering cellulose nitrate (CN) track detectors produce tracks. Therefore track densities produced by given radon activities are increased by such covers to extents predictable from the decay product activities on the overlays. Tracks formed under overlays may etch to larger, more vertical-sided, more easily counted forms. When suspended, uncovered, in air at distances from surfaces greater than the ranges of the alpha particles, three types of CN recorded tracks at the rate (ρ′) of 0.12 tracks cm^?2 (pCi Rn)^?1 1^?1 hr^?1 as predicted by a theoretical expression. In small containers (ρ′) varied with position and container size.     

The relationship of soil 210Po and 210Pb geochemical dispersion patterns to uranium mineralization

²¹⁰Po and ²¹⁰Pb measurements of soils delineated uranium anomalies at three out of four test sites in Ontario, Canada. Measurements were made of ²¹⁰Po in solutions produced by both complete digestion and partial leaching of soil samples. Direct plating of ²¹⁰Po onto metal plates was followed by measuring the alpha activity. Subsequent plating of ²¹⁰Po in-grown from ²¹⁰Pb in solution several months later confirmed the anomalies.The ²¹⁰Po and ²¹⁰Pb anomalies at three of the test sites coincided with ²²⁶Ra and ²²²Rn anomalies. Samples from the fourth uranium occurrence associated with a known ²²²Rn anomaly failed to show either a ²²⁶Ra anomaly on the one hand, or ²¹⁰Po or ²¹⁰Pb anomalies on the other. This suggests that the ²¹⁰Po and ²¹⁰Pb anomalies were probably produced by the decay of ²²⁶Ra contained within secondary dispersion haloes.Although anomalies due to the ²¹⁰Po and ²¹⁰Pb products of ²²²Rn have now been documented, prospecting methods based on their use as direct tracers of the migration paths of ²²²Rn require much further development.     

The relationship of soil Po and Pb geochemical dispersion patterns to uranium mineralization

²¹⁰Po and ²¹⁰Pb measurements of soils delineated uranium anomalies at three out of four test sites in Ontario, Canada. Measurements were made of ²¹⁰Po in solutions produced by both complete digestion and partial leaching of soil samples. Direct plating of ²¹⁰Po onto metal plates was followed by measuring the alpha activity. Subsequent plating of ²¹⁰Po in-grown from ²¹⁰Pb in solution several months later confirmed the anomalies.The ²¹⁰Po and ²¹⁰Pb anomalies at three of the test sites coincided with ²²⁶Ra and ²²²Rn anomalies. Samples from the fourth uranium occurrence associated with a known ²²²Rn anomaly failed to show either a ²²⁶Ra anomaly on the one hand, or ²¹⁰Po or ²¹⁰Pb anomalies on the other. This suggests that the ²¹⁰Po and ²¹⁰Pb anomalies were probably produced by the decay of ²²⁶Ra contained within secondary dispersion haloes.Although anomalies due to the ²¹⁰Po and ²¹⁰Pb products of ²²²Rn have now been documented, prospecting methods based on their use as direct tracers of the migration paths of ²²²Rn require much further development.     

Noble gas study of HIMU and EM ocean island basalts in the Polynesian region

Noble gas isotopes of HIMU and EM ocean island basalts from the Cook-Austral and Society Islands were investigated to constrain their origins. Separated olivine and clinopyroxene (cpx) phenocrysts were used for noble gas analyses. Since samples are relatively old, obtained from the oceanic area and showing chemical zoning in cpx phenocrysts, several tests on sample preparation and gas extraction methods were performed. First, by comparing heating and crushing methods, it has been confirmed that the crushing method is suitable to obtain inherent magmatic noble gases without radiogenic and cosmogenic components which were yielded after eruption, especially for He and Ne analyses. Second, noble gas compositions in the core and the rim of cpx phenocrysts were measured to evaluate the zoning effect on noble gases. The result has been that noble gas concentrations and He and Ne isotope ratios are different between them. The enrichment of noble gases in the rim compared to the core is probably due to fractional crystallization. Difference of He and Ne isotope ratios is explained by cosmogenic effect, and isotope ratios of the trapped component seem to be similar between the rim and the core. Third, leaching test reveals no systematic differences in noble gas compositions between leached and unleached samples.³He/⁴He ratios of HIMU samples in the Cook-Austral Islands are uniform irrespective of phenocryst type (olivine and cpx) and age of samples (10–18 Ma), and lower (average 6.8 R_A) than those of the Pacific MORB. On the other hand, ³He/⁴He of EM samples in the Cook-Austral Islands are similar to MORB values. EM samples in the Society Islands show rather higher ³He/⁴He than MORB. Ne, Kr and Xe isotope ratios are almost atmospheric within analytical uncertainties. ⁴⁰Ar/³⁶Ar are not so high as those of MORB. Anomalous noble gas abundance pattern such as He and Ne depletion and Kr and Xe enrichment relative to atmospheric abundances was observed. Furthermore, Ne/Ar and Kr/Ar show correlation with some trace elemental ratios like La/Yb.Lower ³He/⁴He of HIMU than MORB values requires relatively high time-integrated (U + Th)/³He for the HIMU source, which suggests that the HIMU source was produced from recycled materials which had been once located near the Earth’s surface. Moreover, extreme noble gas abundance pattern and strong correlation of Ne/Ar and Kr/Ar with La/Yb indicate that the HIMU endmember is highly depleted in light noble gases and enriched in heavy noble gases. Such feature is not common to mantle materials and is rather similar to the noble gas abundance patterns of the old oceanic crust and sediment, which supports the model that the HIMU source originates from subducted oceanic crust and/or sediment.If the HIMU source corresponds to the oceanic crust which subducted at 1–2 Ga as suggested by Pb isotope studies, however, the characteristic ³He/⁴He of HIMU (6.8 R_A) would be too high because radiogenic ⁴He produced by U and Th decay should dramatically decrease ³He/⁴He. To overcome this problem, the He open system model is introduced which includes the effects of ⁴He production and diffusion between the HIMU source material and the surrounding mantle. This model favors that the HIMU source resides in the upper mantle, rather than in the lower mantle. Furthermore, this model predicts the thickness of the HIMU source to be in the order of 1 km.In contrast to low and uniform ³He/⁴He character of HIMU, ³He/⁴He of EM are rather variable. Entrainment of upper mantle material and/or a less-degassed component are required to explain the observed ³He/⁴He of EM in the Polynesian area. Participation of the less-degassed component would be related to the “superplume” below the Polynesian region.     

Bismuth and 208Pb microdistributions in enstatite chondrites

Polished sections of 5 enstatite chondrites have been irradiated with 30 MeV ⁴He ions to produce the alpha-radioactive nuclei ²¹¹At and ²¹⁰Po from ²⁰⁹Bi and ²⁰⁸Pb, respectively. The distribution of alpha activity can be mapped, using cellulose nitrate as an alpha track detector, to give the corresponding Bi or Pb distributions in the meteorite. No strong localization of Bi or ²⁰⁸Pb was found; relatively uniform track distributions were observed. In particular, metal or sulfide grains are not enriched in Bi or Pb (relative to bulk), which is in agreement with the predictions of nebular condensation calculations. While the track distributions appear uniform, the results of detailed, track-by-track mappings of the Bi detectors indicate that the Bi is not totally randomly distributed; the statistical fluctuations in the observed track density are different for the cases where the Bi is totally randomly distributed and where the Bi is localized in point sources. Assuming that the Bi in a given sample is localized in identical point sources which are uniformly distributed throughout the sample, the observed relative population densities of clusters (‘stars’) of small numbers of tracks (2–5) corresponds to Bi being localized, with ~90% in grains with about 10^?16g-Bi (~3 × 10⁵Biatoms), and with ~10% in 4 × 10^?14 g-Bi sources. If these are elemental Bi, as predicted theoretically, they are ~ 10² Å and 10³ Å in size, respectively.     

Precise geochronology of phoscorites and carbonatites:: The critical role of U-series disequilibrium in age interpretations

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.     

Zircon M257 ‐ a Homogeneous Natural Reference Material for the Ion Microprobe U‐Pb Analysis of Zircon

We introduce and propose zircon M257 as a future reference material for the determination of zircon U‐Pb ages by means of secondary ion mass spectrometry. This light brownish, flawless, cut gemstone specimen from Sri Lanka weighed 5.14 g (25.7 carats). Zircon M257 has TIMS‐determined, mean isotopic ratios (2s uncertainties) of 0.09100 ± 0.00003 for ²⁰⁶pb/²³⁸U and 0.7392 ± 0.0003 for ²⁰⁷pb/²³⁵U. Its ²⁰⁶pb/²³⁸U age is 561.3 ± 0.3 Ma (unweighted mean, uncertainty quoted at the 95% confidence level); the U‐Pb system is concordant within uncertainty of decay constants. Zircon M257 contains ～ 840 μg g^?1 U (Th/U ～ 0.27). The material exhibits remarkably low heterogeneity, with a virtual absence of any internal textures even in cathodoluminescence images. The uniform, moderate degree of radiation damage (estimated from the expansion of unit‐cell parameters, broadening of Raman spectral parameters and density) corresponds well, within the “Sri Lankan trends”, with actinide concentrations, U‐Pb age, and the calculated alpha fluence of 1.66 × 10¹⁸ g^?1. This, and a (U+Th)/He age of 419 ± 9 Ma (2s), enables us to exclude any unusual thermal history or heat treatment, which could potentially have affected the retention of radiogenic Pb. The oxygen isotope ratio of this zircon is 13.9%o VSMOW suggesting a metamorphic genesis in a marble or calc‐silicate skarn.     

Geothermochronology based on noble gases: III. Migration of radiogenic He in the crystal structure of native metals with applications to their isotopic dating

It was shown that the behavior of ⁴He in native and technical metals is very similar owing to the symmetric and stable electron shells of its atoms, which cannot gain electrons from other atoms or donate their own electrons to metal atoms in a crystal lattice. Therefore, they rapidly migrate toward grain boundaries and dislocations, where they are released as vesicles or He clusters. It was found that the thermal desorption of radiogenic He occurring in the crystal lattice of native metals as gas clusters requires activation energies of 100 and even 180 kcal/mol up to the attainment of the melting temperature of the metal. The frequency factor is several orders of magnitude higher than the limiting value k ₀ ∼ 10¹³ s⁻¹ for the migration of single atoms in the crystal lattice. Near the melting temperature and tens-hundreds degrees above it, the character of the thermal desorption of radiogenic ⁴He changes fundamentally. The migration is strongly accelerated, and sharp narrow peaks appear on the kinetic curves of thermal desorption. A similar phenomenon was observed during the annealing of technical metals and is known as the burst-effect. The destruction of the crystal structure results in the disappearance of helium clusters (vesicles). At the very high temperature, He migrates as individual atoms relatively rapidly from the melt. The activation energy for He thermal desorption and the pre-exponential frequency factor acquire values characteristic of ordinary migration. Such peculiarities of radiogenic He provide unique opportunities for its preservation in the structure of gold and other native metals below their melting temperatures. The rapid advances of (U-Th)/He geochronology is still hampered by the experimentally established extremely heterogeneous distribution of U, He, and, probably, Th in the structure of gold and other natural metals. This difficulty can be circumvented by the development of a method for the determination of the contents of all the mentioned chemical elements in a single aliquot from each sample.     

Pb-Sr-He isotope and trace element geochemistry of the Cape Verde Archipelago

New lead, strontium and helium isotopic data, together with trace element concentrations, have been determined for basalts from the Cape Verde archipelago (Central Atlantic). Isotopic and chemical variations are observed at the scale of the archipelago and lead to the definition of two distinct groupings, in keeping with earlier studies. The Northern Islands (Santo Antão, São Vicente, São Nicolau and Sal) present Pb isotopic compositions below the Northern Hemisphere Reference Line (NHRL) (cf. Hart, 1984), unradiogenic Sr and relatively primitive ⁴He/³He ratios. In contrast, the Southern Islands (Fogo and Santiago) display Pb isotopes above the NHRL, moderately radiogenic Sr and MORB-like helium signatures. We propose that the dichotomy between the Northern and Southern Islands results from the presence of three isotopically distinct components in the source of the Cape Verde basalts: (1) recycled ∼1.6-Ga oceanic crust (high ²⁰⁶Pb/²⁰⁴Pb, low ⁸⁷Sr/⁸⁶Sr and high ⁴He/³He); (2) lower mantle material (high ³He); and (3) subcontinental lithosphere (low ²⁰⁶Pb/²⁰⁴Pb, high ⁸⁷Sr/⁸⁶Sr and moderately radiogenic ⁴He/³He ratios). The signature of the Northern Islands reflects mixing between recycled oceanic crust and lower mantle, to which small proportions of entrained depleted material from the local upper mantle are added. Basalts from the Southern Islands, however, require the addition of an enriched component thought to be subcontinental lithospheric material instead of depleted mantle. The subcontinental lithosphere may stem from delamination and subsequent incorporation into the Cape Verde plume, or may be remnant from delamination just before the opening of the Central Atlantic. Basalts from São Nicolau reflect the interaction with an additional component, which is identified as oceanic crustal material.     

He,Ne, Ar,and C isotope systematics of geothermal emanations in the Lesser Antilles Islands Arc

We present He, Ne, Ar, and C isotope analyses of hydrothermal brines and gases from fumaroles, hot springs, mofettes and hydrothermal exploration drillings on the major islands of the Lesser Antilles Arc. The origin of hydrothermal brines, which have been analyzed also for O and H isotopes, is essentially meteoric-hydrothermal. Air-corrected isotope compositions of helium (2.2 Rc/Ra < ³He/⁴He < 8.6 Rc/Ra) and carbon (−20 < δ¹³C_PDB < +0.5) are variable and require a variety of crustal and magmatic sources. The diversity of δ¹³C_PDB and ³He/CO₂ ratios within individual volcanic centres suggests that crustal sources (e.g., limestone) contaminate magmatic CO₂ en route from high-level magma reservoirs (depth < 15 km) to the surface. A similar contamination may be found for magmatic helium on distal springs. The ³He/⁴He signature of summit fumaroles, thought to reflect the ³He/⁴He signature of high-level magmas, shows a remarkable systematic variation along the arc. In addition, there is a correlation throughout the arc between published Sr, Pb, and Nd isotope signatures of lavas and the ³He/⁴He signatures of summit fumaroles. On the northern islands (Nevis, Montserrat, Guadeloupe, and Dominica) summit fumaroles have the N-MORB signature (³He/⁴He = 8 ± 1 R/Ra), and the isotope signature of lavas is not dissimilar from comparable intra-oceanic arc tholeiites elsewhere. Variable enrichments in radiogenic Sr and Pb have been reported for lavas of individual volcanic centres of the Southern Islands (Martinique, St.Lucia, and Grenada), and summit fumaroles on these centres match these variations by variable radiogenic He-enrichments, i.e., lower ³He/⁴He ratios. This correlation suggests that radiogenic Sr and Pb enrichments of lavas and low ³He/⁴He signatures on summit fumaroles have a common origin, i.e., a terrigenous contaminant derived from the Orinoco depositionary fan. Crustal assimilation is thought to decouple the He isotope system from any other radiogenic isotope system and, therefore, we argue that the observed correlation of He, Sr, Pb, and Nd isotope systems is related to a terrigenous contaminant derived from subducted sediments. Support for this scenario also comes from the matching of low ³He/⁴He ratios and tectonic features of the forearc thought to favor the subduction of forearc sediments.The present study offers a first clue that, under suitable conditions, crustal helium from oceanic sediments might be subducted to the depth of arc magma sources and, possibly, even recycled into the deeper mantle.     

The decay products of rn in etched track radon detection

Precipitation of decay products of atmospheric ²²²Rn in small containers and the effects of their precipitation on alpha-particle-track-measurements of radon activities were studied. From decay curves of decay product activities on surfaces exposed to radon-containing air the ratios ²¹⁴Pb/²¹⁸Po (=r) in the precipitates were determined. From r average ages of precipitating decay products were calculated. Average ages and r were low, indicating rapid precipitation of decay products, and decreased with container size. Activities on exposed surfaces were approximately those expected if decay products precipitate completely and uniformly on the internal surfaces of containers.Decay products precipitated on foils of correct thickness covering cellulose nitrate (CN) track detectors produce tracks. Therefore track densities produced by given radon activities are increased by such covers to extents predictable from the decay product activities on the overlays. Tracks formed under overlays may etch to larger, more vertical-sided, more easily counted forms. When suspended, uncovered, in air at distances from surfaces greater than the ranges of the alpha particles, three types of CN recorded tracks at the rate (ρ′) of 0.12 tracks cm⁻² (pCi Rn)⁻¹ 1⁻¹ hr⁻¹ as predicted by a theoretical expression. In small containers (ρ′) varied with position and container size.     

He-Ar-S-Pb Isotopic Compositions of Pyrite: Constraints on the Source of Ore-forming Materials of the Chengchao Skarn Iron Deposit, SE Hubei Province, Eastern China

The Chengchao iron deposit,the largest high-grade skarn iron deposit in southeastern Hubei Province,contains considerable amounts of magnetite and by-product anhydrite.To obtain better understanding of the ore-formation process,this study carried out He-Ar-S-Pb multi-isotopic analyses on the pyrites formed during two stages of mineralization.The results indicate that the δ~(34)S values(ranging from 14.0‰ to 17.6‰) of pyrites formed from the two stages have no obvious differences,suggesting that they were not derived from a single magmatic sulfur source.The δ~(34)S values of anhydrite mostly range from 21.9‰ to 28.4‰,similar to that of the Middle Triassic sedimentary anhydrite in the Middle-Lower Yangtze River metallogenic belt(MLYRB).The Pb isotopic compositions of the pyrites of both stages are homogeneous,with values of ~(208)Pb/~(204)Pb,~(207)Pb/~(204)Pb,and~(206)Pb/~(204)Pb being 38.006-38.257,15.523-15.556,and 17.806-18.052,respectively,indicating a mixed crust-mantle source.The He-Ar results exhibit different compositions of the two stages:the ~3He/~4He(R/Ra) and ~(40)Ar/~(36)Ar values for the early-stage pyrite are 0.46-0.63 and 311-322,respectively,whereas the values for late-stage pyrite are 0.23-0.34 and 305-361,respectively.Both stages of pyrites indicate the multiple sources of the ore-forming fluids,with decreasing amount of magmatic water and increasing amount of modified meteoric water(MASW) during fluid evolution.The Triassic evaporites played an important role in the mineralization process.     

Deposition of uraninite in microfissures of uranothorianite

Deposition of uraninite in microfissures of uranothorianite crystals, in a proluvialdeluvial placer of titaniferous magnetite (with Pb and many other impurities) is understandably the result of self-oxidation of U⁴⁺ to U⁶⁺ in the mineral (e.g. by radiogenic oxygen produced by decay of thorium in the presence of lead), its outward migration (as by leaching), and then its partial reduction, UO₃ to UO₂, deposition, and preservation, under certain conditions, as in the Arctic or Japan.     

Carbon and Noble Gas Isotopes in the Tengchong Volcanic Geothermal Area, Yunnan, Southwestern China

Carbon and noble gas isotope analyses are reported for bubbling gas samples from the Tengchong volcanic geothermal area near the Indo-Eurasian suture zone. All samples contain a resolvable component of mantle-derived 3He. Occurrence of mantle-derived 3He coincides with surface volcanism. However, 3He occurs over a larger geographic areathan do surface volcanics. δ13C values for CO2 and CH4 vary from -33.4‰ to 1.6 ‰ and from -52.8‰ to -2.8‰, respectively. He and C isotope systematics indicate that CO2 and CH4 in the CO2-rich gases originated predominantly from magmatic component mixed with crustal CO2 produced from carbonate. However, breakdown of organic matter and near-surface processes accounts for the CH4 and CO2 in N2-rich gases. 3He/4He ratio distribution pattern suggests that mantle-derived He and heat sources of high-temperature system in central Tengchong originate from a hidden magma reservoir at subsurface. CO2-rich gases with the highest 3He/4He ratio (5.2 Ra) may be representative of the     

Noble Gas and Stable Isotopic Constraints on the Origin of the Ag–Cu Polymetallic Ore Deposits in the Baiyangping Area,Yunnan Province,SW China

The Lanping basin, Yunnan province, SW China, is located at the juncture of the Eurasian and Indian Plates in the eastern part of the Tibetan Plateau. The Lanping basin, in the Sanjiang Tethyan metallogenic province, is a significant Cu–Ag–Zn–Pb mineralized belt in China that includes the largest sandstone‐hosted Zn–Pb deposit in the world, the Jinding deposit, as well as several Ag–Cu deposits (the Baiyangping and Jinman deposits). These deposits, with total reserves of over 16.0 Mt Pb + Zn, 0.6 Mt Cu, and 7,000 t Ag, are mainly hosted in Meso‐Cenozoic clastic rocks and are dominantly controlled by two Cenozoic thrust systems developed in the western and eastern segments of the basin. The Baiyangping, Babaoshan, and Hetaoqing ore deposits are representative of the epithermal base metal deposits in the Lanping basin. The microthermometric data show that the ore‐forming fluids for these deposits were low temperature (110–180 °C) and had bimodal distribution of salinity at moderate and mid to high salinities (approximately 2–8 wt.% and 18–26 wt.% NaCl equivalent). The C and O isotope data indicate that the ore‐forming fluids were related to hot basin brines. We present new He and Ar isotope data on volatiles released from fluid inclusions contained in sulfides and in barite in these three deposits. ³He/⁴He ratios of the ore‐forming fluids are 0.01 to 0.14 R/Ra with a mean of 0.07 Ra (where R is the ³He/⁴He ratio and Ra is the ratio for atmospheric helium). This mean value is intermediate to typical ³He/⁴He ratios for the crust (R/Ra = 0.01 to 0.05) and the ratio for air‐saturated water (R/Ra = 1). The mean ratio is also significantly lower than the ratios found for mantle‐derived fluids (R/Ra = 6 to 9). The ⁴⁰Ar/³⁶Ar ratios of the ore‐forming fluids range from 298 to 382 with a mean of 323. This value is slightly higher than that for the air‐saturated water (295.5). The ³He/⁴He ratios of fluids from the fluid inclusions imply that the ore‐forming fluid for the Baiyangping, Babaoshan, and Hetaoqing deposits was derived from the crust and that any mantle‐derived He was negligible. The content of the radiogenic Ar ranges between 0.2 to 20.4%, and the proportion of air‐derived ⁴⁰Ar averages 94.1%. This indicates that atmospheric Ar was important in the formation of these deposits but that some radiogenic ⁴⁰Ar was derived from crustal rocks. Based on these observations coupled with other geochemical evidence, we suggest that the ore‐forming fluids responsible for the formation of the Ag–Cu–Pb–Zn polymetallic ore deposits in the Baiyangping area of the Lanping basin were mainly derived from crustal fluids. The fluids may have mixed with some amount of air‐saturated water, but there was no significant involvement of mantle‐derived fluids.     

（U-Th）/He定年——低温热年代学研究的一种新技术

近年来（U-Th）/He定年方法在技术和低温热年代学应用上的优势吸引人们以此开展构造、地形地貌演化等的研究；与裂变径迹、K Ar、Ar Ar等定年方法的比较，该方法是有效的；人们研究了温度及矿物粒径对He扩散的影响，确定了校正方法。（U-Th）/He的封闭温度低于其它体系（磷灰石的仅为75℃±）；有质谱仪只需数十毫克样品就能获得 U、Th、He含量；有较裂变径迹法快速、省样、省力的优点；该技术虽还有待完善，但仍不失为开展低温热年代学和低温热演化研究的潜在有效方法。     

Reassessing the uranium decay constants for geochronology using ID-TIMS U-Pb data

As the internal precision of radiometric dates approaches the 0.1% level, systematic biases between different methods have become apparent. Many workers have suggested that calibrating other decay constants against the U-Pb system is a viable solution to this problem. We test this assertion empirically and quantitatively by analyzing U-Pb systematics of zircon and xenotime on the single- to sub-grain scale by high-precision ID-TIMS geochronology on 11 rock samples ranging from 0.1 to 3.3 Ga. Large statistically equivalent datasets give ²⁰⁷Pb/²⁰⁶Pb dates that are systematically older than ²⁰⁶Pb/²³⁸U dates by ∼0.15% in Precambrian samples to as much as ∼3.3% in Mesozoic samples, suggesting inaccuracies in the mean values of one or both of the U decay constants. These data are used to calculate a ratio of the U decay constants that is lower than the accepted ratio by 0.09% and is a factor of 5 more precise. Four of the samples are used to augment existing data from which the U-Pb and ⁴⁰Ar/³⁹Ar systems can be compared. The new data support most previous observations that U-Pb and ²⁰⁷Pb/²⁰⁶Pb dates are older than ⁴⁰Ar/³⁹Ar by ?1%, though scatter in the amount of offset in samples as a function of age suggests that the bias is not entirely systematic, and may incorporate interlaboratory biases and/or geologic complexities. Studies that calibrate other decay schemes against U-Pb should include an assessment of inaccuracies in the U decay constants in addition to other systematic biases and non-systematic geologic uncertainty.     

Mantle heat drives hydrothermal fluids responsible for carbonate-hosted base metal deposits: evidence from 3He/4He of ore fluids in the Irish Pb-Zn ore district

There is little consensus on whether carbonate-hosted base metal deposits, such as the world-class Irish Zn + Pb ore field, formed in collisional or extensional tectonic settings. Helium isotopes have been analysed in ore fluids trapped in sulphides samples from the major base metal deposits of the Irish Zn-Pb ore field in order to quantify the involvement of mantle-derived volatiles that require melting to be realised, as well as test prevailing models for the genesis of the ore fields. ³He/⁴He ratios range up to 0.2 R _a, indicating that a small but clear mantle helium contribution is present in the mineralising fluids trapped in galena and marcasite. Sulphides from ore deposits with the highest fluid inclusion temperatures (~200 °C) also have the highest ³He/⁴He (>0.15 R _a). Similar ³He/⁴He are recorded in fluids from modern continental regions that are undergoing active extension. By analogy, we consider that the hydrothermal fluids responsible for the carbonate-hosted Irish base metal mineralization circulated in thinned continental crust undergoing extension and demonstrate that enhanced mantle heat flow is ultimately responsible for driving fluid convection.