Evidence for anthropogenic ¹⁴C-enrichment in estuarine waters adjacent to the North Sea

[1] The isotopic composition (d13C and D14C) of high molecular weight dissolved organic carbon (HMW DOC) was studied in the Tyne and Tweed estuaries, NE England. Despite significant removal of terrigenous HMW DOC in the low salinity regions (S < 15), D14C remained modern with little variation around 115%. This lack of apparent age discrimination was attributed to either non-oxidative removal or the absence of a significant proportion of old refractory C in the HMW DOC pool. At S < 15, we observed seaward increases in d13C and D14C. With no documented local 14C inputs, we attributed non-bomb related 14C-enrichment at S < 15 to a possible ‘lingering effect’ of distal anthropogenic sources in near-coastal North Sea HMW DOC. Given the global distribution of potential sources, we propose that anthropogenic 14C should be considered in assigning ages of DOC pools in near-coastal waters and suggest its possible use as a tracer for DOC transformations

Lessons from a large scale deployment of DGT in the Seine basin

Diffusive Gradient in Thin film (DGT) is a speciation technique now commonly used in the scientific literature to assess metallic contamination in water. However applications usually take place in a same watercourse or in neighbouring sites. We propose here to present the first results of a large scale deployment of DGTs. The main objective of the project, which is supported by the French water agency of the Seine-Normandie basin, is to evaluate the potential of passive samplers as monitoring tools. DGT devices were deployed in 45 sites, on 30 locations in the entire Seine river basin. The sampling area was 500 km long and 200 km wide around Paris. The total sampling period lasted over the whole 2009 year. Restricted gels of 0.78 were used to measure labile Cd, Cr, Co, Cu, Mn, Ni, Pb and Zn. In parallel, raw and filtered water samples were collected to measure total and dissolved metals. General physico-chemical parameters were also measured. The whole set of measurements constitute a rich dataset including large and small rivers, and reference as well as impacted sites. The results first allow us to draw a map of total, dissolved and labile metal concentrations, representing the spatial variability of metal contamination in the Seine basin. Moreover, considering the temporal variability, different behaviours, depending on the metal, can be identified. The large scale deployment of DGT in the Seine river basin was successful: all the samples have been interpreted and are exploitable, whereas the dissolved metal samples are sometimes under the detection limit. We have then built a representative data set on the water contamination in labile metal of an urban impacted basin. The results are also interpreted as labile percentage, showing the operationally possible values of lability in contrasted environmental conditions. A first approach of the factors influencing the lability highlights the significance of the nature of the organic matter to interpret the lability of the metals

Superconductivity in the New Platinum Germanides MPt4Ge12 (M = Rare-earth and Alkaline-earth Metals) with Filled Skutterudite Structure

New germanium-platinum compounds with the filled-skutterudite crystal structure were synthesized. The structure and composition were investigated by X-ray diffraction and microprobe analysis. Magnetic susceptibility, specific heat, and electrical resistivity measurements evidence superconductivity in LaPt4Ge12 and PrPt4Ge12 below 8.3K. The parameters of the normal and superconducting states were established. Strong coupling and a crystal electric field singlet groundstate is found for the Pr compound. Electronic structure calculations show a large density of states at the Fermi level. Similar behavior with lower T_c was observed for SrPt4Ge12 and BaPt4Ge12.Comment: RevTeX, 4 figures, submitted to Physical Review Letters July 12, 200

Open ocean carbon monoxide photo-production

Sunlight-initiated photolysis of chromophoric dissolved organic matter (CDOM) is the dominant source of carbon monoxide (CO) in the open-ocean. A modelling study was conducted to constrain this source. Spectral solar irradiance was obtained from two models (GCSOLAR and SMARTS2). Water-column CDOM and total light absorption were modelled using spectra collected along a Meridional transect of the Atlantic ocean using a 200-cm pathlength liquid waveguide UV-visible spectrophotometer. Apparent quantum yields for the production of CO (AQYCO) from CDOM were obtained from a parameterisation describing the relationship between CDOM light absorption coefficient and AQYCO and the CDOM spectra collected. The sensitivity of predicted rates to variations in model parameters (solar irradiance, cloud cover, surface-water reflectance, CDOM and whole water light absorbance, and AQYCO was assessed. The model\u27s best estimate of open-ocean CO photoproduction was 47 +/- 7 Tg CO-C yr-1, with lower and upper limits of 38 and 84 Tg CO-C yr-1, as indicated by sensitivity analysis considering variations in AQYs, CDOM absorbance, and spectral irradiance. These results represent significant constraint of open-ocean CO photoproduction at the lower limit of previous estimates. Based on these results, and their extrapolation to total photochemical organic carbon mineralisation, we recommend a downsizing of the role of photochemistry in the open-ocean carbon cycle. (c) 2006 Elsevier Ltd. All rights reserved

Nitrous oxide and methane in the Atlantic Ocean between 50 degrees North and 52 degrees South: Latitudinal distribution and sea-to-air flux

We discuss nitrous oxide (N2O) and methane (CH4) distributions in 49 vertical profiles covering the upper 300 m of the water column along two 13,500 km transects between 50°N and 52°S during the Atlantic Meridional Transect (AMT) programme (AMT cruises 12 and 13). Vertical N2O profiles were amenable to analysis on the basis of common features coincident with Longhurst provinces. In contrast, CH4 showed no such pattern. The most striking feature of the latitudinal depth distributions was a well-defined “plume” of exceptionally high N2O concentrations coincident with very low levels of CH4, located between 23.5°N and 23.5°S; this feature reflects the upwelling of deep waters containing N2O derived from nitrification, as identified by an analysis of N2O, apparent oxygen utilization (AOU) and NO3-, and presumably depleted in CH4 by bacterial oxidation. Sea-to-air emissions fluxes for a region equivalent to 42% of the Atlantic Ocean surface area were in the range 0.40–0.68 Tg N2O yr-1 and 0.81–1.43 Tg CH4 yr-1. Based on contemporary estimates of the global ocean source strengths of atmospheric N2O and CH4, the Atlantic Ocean could account for 6–15% and 4–13%, respectively, of these source totals. Given that the Atlantic Ocean accounts for around 20% of the global ocean surface, on unit area basis it appears that the Atlantic may be a slightly weaker source of atmospheric N2O than other ocean regions but it could make a somewhat larger contribution to marine-derived atmospheric CH4 than previously thought

High spin polarization in the ferromagnetic filled skutterudites KFe4Sb12 and NaFe4Sb12

The spin polarization of ferromagnetic alkali-metal iron antimonides KFe4Sb12 and NaFe4Sb12 is studied by point-contact Andreev reflection using superconducting Nb and Pb tips. From these measurements an intrinsic transport spin polarization Pt of 67% and 60% for the K and Na compound, respectively, is inferred which establishes these materials as a new class of highly spin polarized ferromagnets. The results are in accord with band structure calculations within the local spin density approximation (LSDA) that predict nearly 100% spin polarization in the density of states. We discuss the impact of calculated Fermi velocities and spin fluctuations on Pt.Comment: Pdf file with fi

Low temperature ferromagnetic properties of the diluted magnetic semiconductor Sb2-xCrxTe3

We report on magnetic and electrical transport properties of Sb2-xCrxTe3 single crystals with 0 <= x <= 0.095 over temperatures from 2 K to 300 K. A ferromagnetic state develops in these crystals at low temperatures with Curie temperatures that are proportional to x (for x > 0.014), attaining a maximum value of 20 K for x = 0.095. Hysteresis below TC for applied field parallel to the c-axis is observed in both magnetization and Hall effect measurements. Magnetic as well as transport data indicate that Cr takes the 3+ (3d3) valence state, substituting for antimony in the host lattice structure, and does not significantly affect the background hole concentration. Analysis of the anomalous Hall effect reveals that skew scattering is responsible for its presence. These results broaden the scope of ferromagnetism in the V2-VI3 diluted magnetic semiconductors (DMS) and in ferromagnetic DMS structures generallyComment: 24 pages, 5 figures, submitted to PR

Defect structure of Sb2−xCrxTe3 single crystals

Single crystals of Sb2Te3 doped with Cr (cCr=0–6×1020 cm-3) were prepared by the Bridgman method. The measurements of the Hall coefficient reveal a nonmonotonous dependence of hole concentrations on the Cr content in the crystal. The hole concentration decreases at low content of Cr, while at higher content of Cr it increases again. However, according to magnetic measurements, Cr atoms enter the structure and form uncharged substitutional defects CrSb×, which cannot affect the free carrier concentration directly. The observed dependence can be elucidated by means of a point defect model. The model is based on an assumption that defect structure of Sb2Te3 can be treated as hybrid Schottky and antisite defect disorder. Thus, we assume an interaction of CrSb× with the most populated native defects in the structure—antisite defects SbTe-1 and vacancies in the Te sublattice VTe+2