| 1. |
- Berthet, Gwenaël, et al.
(författare)
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Impact of a moderate volcanic eruption on chemistry in the lower stratosphere : balloon-borne observations and model calculations
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:3, s. 2229-2253
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Tidskriftsartikel (refereegranskat)abstract
- The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at midlatitudes. Since then, only moderate but recurrent volcanic eruptions have modulated the stratospheric aerosol loading and are assumed to be one cause for the reported increase in the global aerosol content over the past 15 years. This particularly enhanced aerosol context raises questions about the effects on stratospheric chemistry which depend on the latitude, altitude and season of injection. In this study, we focus on the midlatitude Sarychev volcano eruption in June 2009, which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) into a lower stratosphere mainly governed by high-stratospheric temperatures. Together with in situ measurements of aerosol amounts, we analyse high-resolution in situ and/or remote-sensing observations of NO2, HNO3 and BrO from balloon-borne infrared and UV-visible spectrometers launched in Sweden in August-September 2009. It is shown that differences between observations and three-dimensional (3-D) chemistry-transport model (CTM) outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km altitude. Good measurement-model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of similar to 45% and increases of similar to 11% in NO2 and HNO3 amounts respectively over the August-September 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (similar to 22 %) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2 hydrolysis. We show that the chlorine partitioning is significantly controlled by enhanced BrONO2 hydrolysis. However, simulated effects of the Sarychev eruption on chlorine activation are very limited in the high-temperature conditions in the stratosphere in the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated chemical ozone loss due to the Sarychev aerosols is low with a reduction of -22 ppbv (-1.5 %) of the ozone budget around 16 km. This is at least 10 times lower than the maximum ozone depletion from chemical processes (up to -20 %) reported in the Northern Hemisphere lower stratosphere over the first year following the Pinatubo eruption. This study suggests that moderate volcanic eruptions have limited chemical effects when occurring at midlatitudes (restricted residence times) and outside winter periods (high-temperature conditions). However, it would be of interest to investigate longer-lasting tropical volcanic plumes or sulfur injections in the wintertime low-temperature conditions.
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| 2. |
- Björkman, Mats P., et al.
(författare)
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Nitrate dry deposition in svalbard
- 2013
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Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 65, s. 19071-
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Tidskriftsartikel (refereegranskat)abstract
- Arctic regions are generally nutrient limited, receiving an extensive part of their bio-available nitrogen from the deposition of atmospheric reactive nitrogen. Reactive nitrogen oxides, as nitric acid (HNO3) and nitrate aerosols (p-NO3), can either be washed out from the atmosphere by precipitation or dry deposited, dissolving to nitrate (NO3-). During winter, NO3- is accumulated in the snowpack and released as a pulse during spring melt. Quantification of NO3- deposition is essential to assess impacts on Arctic terrestrial ecology and for ice core interpretations. However, the individual importance of wet and dry deposition is poorly quantified in the high Arctic regions where in-situ measurements are demanding. In this study, three different methods are employed to quantify NO3- dry deposition around the atmospheric and ecosystem monitoring site, Ny-Alesund, Svalbard, for the winter season (September 2009 to May 2010): (1) A snow tray sampling approach indicates a dry deposition of -10.27 +/- 3.84 mg m(-2) (+/- S.E.); (2) A glacial sampling approach yielded somewhat higher values -30.68 +/- 12.00 mg m(-2); and (3) Dry deposition was also modelled for HNO3 and p-NO3 using atmospheric concentrations and stability observations, resulting in a total combined nitrate dry deposition of -10.76 +/- 1.26 mg m(-2). The model indicates that deposition primarily occurs via HNO3 with only a minor contribution by p-NO3. Modelled median deposition velocities largely explain this difference: 0.63 cm s(-1) for HNO3 while p-NO3 was 0.0025 and 0.16 cm s(-1) for particle sizes 0.7 and 7 mm, respectively. Overall, the three methods are within two standard errors agreement, attributing an average 14% (total range of 2-44%) of the total nitrate deposition to dry deposition. Dry deposition events were identified in association with elevated atmospheric concentrations, corroborating recent studies that identified episodes of rapid pollution transport and deposition to the Arctic.
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| 3. |
- Björkman, Mats P., 1978, et al.
(författare)
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Nitrate postdeposition processes in Svalbard surface snow
- 2014
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Ingår i: Journal of Geophysical Research - Atmospheres. - 0148-0227 .- 2156-2202 .- 2169-897X .- 2169-8996. ; 119:22
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Tidskriftsartikel (refereegranskat)abstract
- The snowpack acts as a sink for atmospheric reactive nitrogen, but several postdeposition pathways have been reported to alter the concentration and isotopic composition of snow nitrate with implications for atmospheric boundary layer chemistry, ice core records, and terrestrial ecology following snow melt. Careful daily sampling of surface snow during winter (11-15 February 2010) and springtime (9 April to 5 May 2010) near Ny-Ålesund, Svalbard reveals a complex pattern of processes within the snowpack. Dry deposition was found to dominate over postdeposition losses, with a net nitrate deposition rate of (0.6+/-0.2) (my) molm 2 d 1 to homogeneous surface snow. At Ny-Ålesund, such surface dry deposition can either solely result from long-range atmospheric transport of oxidized nitrogen or include the redeposition of photolytic/bacterial emission originating from deeper snow layers. Our data further confirm that polar basin air masses bring 15 N-depleted nitrate to Svalbard, while high nitrate (delta) (18O) values only occur in connection with ozone-depleted air, and show that these signatures are reflected in the deposited nitrate. Such ozone-depleted air is attributed to active halogen chemistry in the air masses advected to the site. However, here the Ny-Ålesund surface snow was shown to have an active role in the halogen dynamics for this region, as indicated by declining bromide concentrations and increasing nitrate (delta) (18O), during high BrO (low-ozone) events. The data also indicate that the snowpack BrO-NO x cycling continued in postevent periods, when ambient ozone and BrO levels recovered.
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