Abstract: The cosmogenic radionuclide 35S (half life ∼87 d) exists in both 35SO2 gas and 35SO42− aerosol phase in the atmosphere. Cosmogenic 35S fulfils a unique niche in that it has an ideal half-life for use as a tracer of atmospheric processes, possesses a gas phase precursor and undergoes gas to particle conversion, providing a chronometer that complements other measurements of radiogenic isotopes of different half lives and chemical properties. Based on radiogenic 35S measurements and concomitant model calculations, we demonstrate that 35S is a unique tracer to understand stratospheric-tropospheric air mass transport dynamics and the atmospheric oxidation capacity on a short time scale. Reported are the first measurements of 35S contained in SO42− aerosols (bulk and size aggregated) at Antarctica. 35SO42− concentrations at Dome C and Dumont D'Urville exhibit summer maxima and winter minima with a secondary winter peak. Higher oxidative capacity of the atmosphere and long range transport of mid latitude air increases 35SO42− activity in summer whereas a lack of air mass mixing coupled with low oxidant concentration in winter significantly decreases 35SO42− activity. A 3% contribution from stratospheric 35SO42− into the free troposphere during stratosphere-troposphere air mass mixing accounts for the secondary winter 35SO42− peak. In the future, this work will be extended to 35S activity measurements of both gas and aerosol phases to further understand gas to particle conversion, vortex dynamics and trace polar stratospheric cloud sedimentation frequency.

Abstract: Atmospheric nitrogen oxides (NOx =NO+ NO2) play a pivotal role in the cycling of reactive nitrogen (ultimately deposited as nitrate) and the oxidative capacity of the atmosphere. Combined measurements of nitrogen and oxygen stable isotope ratios of nitrate collected in the Arctic atmosphere were used to infer the origin and fate of NOx and nitrate on a seasonal basis. In spring, photochemically driven emissions of reactive nitrogen from the snowpack into the atmosphere make local oxidation of NOx by bromine oxide the major contributor to the nitrate budget. The comprehensive isotopic composition of nitrate provides strong constraints on the relative importance of the key atmospheric oxidants in the present atmosphere, with the potential for extension into the past using ice cores.

Abstract: The reconstruction of past volcanism from glaciological archives is based on the measurement of sulfate concentrations in ice. This method does not allow a proper evaluation of the climatic impact of an eruption owing to the uncertainty in classifying an event between stratospheric or tropospheric. This work develops a new method, using anomalous sulfur isotope composition of volcanic sulfate in order to identify stratospheric eruptions over the last millennium. The advantages and limits of this new method are established with the examination of the 10 largest volcanic signals in ice cores from Dome C and South Pole, Antarctica. Of the 10, seven are identified as stratospheric eruptions. Among them, three have been known to be stratospheric (Tambora, Kuwae, the 1259 Unknown Event) and they exhibit anomalous sulfur isotope compositions. Three unknown events (circa 1277, 1230, 1170 A.D.) and the Serua eruption have been identified as stratospheric eruptions, which suggests for the first time that they could have had significant climatic impact. However, the Kuwae and the 1259 Unknown Event stratospheric eruptions exhibit different anomalous sulfur isotope compositions between South Pole and Dome C samples. Differences in sulfate deposition and preservation patterns between the two sites can help explain these discrepancies. This study shows that the presence of an anomalous sulfur isotope composition of volcanic sulfate in ice core indicates a stratospheric eruption, but the absence of such composition does not necessarily lead to the conclusion of a tropospheric process because of differences in the sulfate deposition on the ice sheet.

Abstract: EGU General Assembly, poster, Abstract EGU2009-8637