L'archivage des activités humaines par les neiges et glaces polaires : le cas du plomb

The investigation of the occurrence of lead in dated snow and ice from Greenland and Antarctica has played a major role in our understanding of the history of the pollution of the atmosphere of our planet by this metal. Such studies have however proved to be very demanding, mainly because of the extreme purity of polar snow and ice. Reliable measurements can be obtained only if ultra-clean and highly sensitive procedures are used, as pioneered by Clair Patterson. The Greenland data show evidence of large-scale pollution of the atmosphere of the Northern Hemisphere for lead as early as two millennia ago during Greco–Roman times, especially because of mining and smelting activities in southern Spain. It peaked at the end of the 1960s, with lead concentrations in snow about 200 times higher than natural values, before declining during recent times because of the fall in the use of leaded gasoline. Lead pollution in Antarctica was already significant at the end of the 19th century as a consequence of whaling activities, the traffic of coal-powered ships crossing the Cape Horn, and mining activities in South America, South Africa and Australia. After declining because of the opening of the Panama Canal, the great economic depression and World War II, it reached a maximum during the 1980s, with lead concentrations 20 times higher than natural values. Other studies focus on past natural variations of lead in ancient ice dated from the last climatic cycles. To cite this article: C. Boutron et al., C. R. Geoscience 336 (2004).     

Concentration, isotopic composition, and sources of lead in Southern Ocean air during 1999/2000, measured at the Cape Grim Baseline Air Pollution Station, Tasmania

Southern Ocean aerosols were collected at the Cape Grim Baseline Air Pollution Station from onshore air under baseline conditions between February 1999 and April 2000. Thermal ionization techniques (TIMS) and isotope dilution mass spectrometry (IDMS) were used to measure the isotopic composition and concentration of lead in the air giving concentrations as low as 0.6 ± 0.1 pg · m⁻³. Air collected under baseline conditions for 12 months (May 1999-April 2000) yielded an overall lead concentration of 11.0 ± 0.2 pg · m⁻³ and isotopic composition of ²⁰⁶Pb/²⁰⁷Pb = 1.154, ²⁰⁸Pb/²⁰⁷Pb = 2.387 and ²⁰⁶Pb/²⁰⁴Pb = 17.93. The range in isotopic ratios was consistent with the mixing of lead from major population centers in the Southern Hemisphere in the mid to high latitudes, except for the presence of highly radiogenic lead in some samples. Contributions from radiogenic lead of up to ∼0.8% were observed. Three periods with the highest percentage contribution of radiogenic lead (>0.5%) were investigated in more detail, and 4-d back-trajectories and radon concentrations were used to help identify the sources. The sources are probably associated with the mining and processing of uranium rich ores in southern Africa and possibly South Australia.     

The isotopic composition and elemental abundance of lutetium in meteorites and terrestrial samples and the 176Lu cosmochronometer

The isotopic composition of lutetium has been measured in a range of terrestrial and meteoritic materials using solid-source mass spectrometric techniques. The meteoritic and terrestrial isotopic abundances are identical within experimental errors. The absolute ¹⁷⁵Lu/¹⁷⁶Lu ratio as determined in this work is 37.36 ± 0.07 at the 95% confidence level. On the basis of this measurement the atomic weight of lutetium has been calculated to be 174.967 ± 0.002, which is in good agreement with the currently accepted figure of 174.97 ± 0.01.Using the stable isotope dilution technique the abundance of lutetium has been determined in 25 stone, 1 stony-iron and 8 iron meteorites, and in 12 standard rocks, with an accuracy of ±5% at the 95% confidence level. In general, there is good agreement between this work and other published data.The ¹⁷⁶Lu-¹⁷⁶Hf pair has been proposed as an s process nucleocosmochronometer, because of the long half-life of ¹⁷⁶Lu and the unique fact that both are s process isobars. The isotopic and elemental abundances of lutetium as measured in this work have been used with published nuclear data to estimate the mean age of s process nucleosynthesis for this isobaric pair, using the Schramm-Wasserburg formalism. The mean age cannot be accurately determined at the present time because of the lack of 30 keV neutron capture cross-section data for s only process nuclides and an accurate measurement of the branching ratio of ¹⁷⁵Lu + n. However, it is possible to place constraints on the nuclear parameters in this mass region using a reasonable s process chronology based on the decay of ¹⁷⁶Lu.     

Mass spectrometric isotope dilution analyses of cadmium in standard rocks

Cadmium has been determined in a range of silicate rock standards using the stable isotope dilution technique incorporating solid source mass spectrometry. Our recommended values are, in general, lower than the previously reported data.     

Seasonal variations in the origin of lead in snow at Dye 3, Greenland

The isotopic composition and concentration of lead has been measured in fresh and slightly aged snow collected at Dye 3 in southern Greenland during one full year. The lead concentration displayed large variations ranging from 14–3016 pg/g in April (spring) to 3–6 pg/g in September (summer) while the isotopic ratios changed in regular manner during the year. The ²⁰⁶Pb/²⁰⁷Pb ratios were 1.15 from spring to mid-summer snow, and increased in late summer to early autumn, reaching 1.20 in winter. These isotopic data indicate that the lead in the autumn to winter snow originated in North America, while that in spring to mid-summer snow is from Eurasia.     

The Oklo natural reactor: Cumulative fission yields and retentivity of the symmetric mass region fission products

Solid source mass spectrometry has been used to determine the relative cumulative fission yields of five elements in three samples of uranium ore from reactor zones in the Oklo mine site. Eighteen fission chains covering the mass range from105 ≤ A ≤ 130 have been measured for Pd, Ag, Cd, Sn and Te. These measurements have enabled a number of nuclear parameters to be calculated including the relative proportions of²³⁵U,²³⁸U and²³⁹Pu involved in the fission process.The concentration of the five elements in the Oklo samples have also been measured using the stable isotope dilution technique. These values have then been compared to the estimates of the amount of these elements produced by fission under the conditions that are appropriate to the three samples. This procedure enables the retentivity of the elements in the reactor zones to be evaluated. Our work confirms the fact that Pd and Te are retained almost in their entirety in the samples, whereas the other three elements have been partially lost from the reactor site. Almost all the Cd fission products have been lost, and more than 50% of the Ag and Sn fission-produced material has been removed.     

The abundance of cadmium and zinc in meteorites

A stable isotope dilution technique using solid source mass spectrometry has been used to accurately determine Cd and Zn in a wide range of materials. The abundance of Cd has been determined in 19 iron, 28 stone and 1 stony-iron meteorites, together with a number of other samples. The abundance of Zn has also been determined for most of these samples. This has enabled the relationship between Cd and Zn to be examined in iron and stone meteorites. The abundance pattern of Zn in iron meteorites supports the existence of chemical groups.     

Deficiencies in the classical model of s-process nucleosynthesis

Abstract— The classical model of s-process nucleosynthesis, based on the concept of a steady neutron flux under astrophysical conditions pertaining to the He-burning phase of red giant stars, has successfully described observed isotopic abundances and provided information on the physical conditions of the s-process environment. Because most of the isotopes on the s-process path are stable, their relevant nuclear parameters can be measured in the laboratory so that as more accurate elemental abundance and neutron capture cross-section data have become available, the classical model has been tested under increasingly stringent conditions. Accurate determinations of the neutron capture cross sections at appropriate astrophysical conditions for the Ba isotopes have shown that the abundance of the s-only isotope ¹³⁶Ba is under-produced by ～20% according to the classical model. This paper describes the accurate assessment of the meteoritic abundance of Ba by the stable isotope dilution mass spectrometric technique, based on the Cl carbonaceous chondrites Orgueil and Ivuna. Repeated analyses of these two Cl chondrites give an abundance that is identical to the presently accepted solar system value for Ba within experimental errors, which indicates a deficiency in the classical model. When combined with similar data for the s-only nuclides ¹¹⁶Sn and ¹⁴²Nd, it is apparent that the classical model, having served a valuable function for many years, must be replaced by stellar models that more accurately reflect the dynamic nature of the He-burning phase in red giant stars, in particular, during the thermal pulses of low-mass asymptotic giant branch (AGB) stars.     

A Model for Understanding the Effects of Sediment Dynamics on Oyster Reef Development

Previous field studies have demonstrated that sedimentation is an important factor that can limit oyster reef growth and restoration success. High relief reefs are more productive and resilient than low relief reefs, in part, because increasing reef height reduces sedimentation and enhances oyster growth. In this study, we investigated the relationship between initial reef height and reef development using a simple model. The model contains three coupled differential equations that describe changes in oyster volume, shell volume, and sediment volume per unit area of reef with time. The model was used to investigate how parameters such as flow speed, sediment grain size, and food concentration affect reef survival and final reef height. Whether or not a reef survives depends primarily on the shape of the sediment concentration profile relative to the initial reef height. Over a long time period, three different steady-state reef heights are possible, depending on the environmental parameters and initial reef height: (1) If growth outpaces sedimentation, the reef achieves the maximum possible height, which is independent of sedimentation parameters; (2) if deposition outpaces growth and the shear stress does not exceed the critical shear stress, the reef is buried in sediment and dies; and (3) if deposition outpaces growth and the shear stress exceeds the critical shear stress, a reduced steady-state height is achieved that depends on both growth and sedimentation parameters. The model can be used to assess the ways in which measurable environmental parameters affect reef restoration success.