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Two consecutive cruises in the Weddell Sea, Antarctica, in winter 2013 provided the first direct observations of sea salt aerosol (SSA) production from blowing snow above sea ice, thereby validating a model hypothesis to account for winter time SSA maxima in polar regions not explained otherwise. Blowing or drifting snow always lead to increases in SSA during and after storms. Observed aerosol gradients suggest that net production of SSA takes place near the top of the blowing or drifting snow layer. The observed relative increase of SSA concentrations with wind speed suggests that on average the corresponding aerosol mass flux during storms was equal or larger above sea ice than above the open ocean, demonstrating the importance of the blowing snow source for SSA in winter and early spring. For the first time it is shown that snow on sea ice is depleted in sulphate relative to sodium with respect to sea water. Similar depletion observed in the aerosol suggests that most sea salt originated from snow on sea ice and not the open ocean or leads, e.g. on average 93 % during the 8 June and 12 August 2013 period. A mass budget calculation shows that sublimation of snow even with low salinity (< 1 psu) can account for observed increases of atmospheric sea salt from blowing snow. Furthermore, snow on sea ice and blowing snow showed no or small depletion of bromide relative to sodium with respect to sea water, whereas aerosol at 29 m was enriched suggesting that SSA from blowing snow is a source of atmospheric reactive bromine, an important ozone sink, with bromine loss taking place preferentially in the aerosol phase between 2 and 29 m above the sea ice surface. Evaluation of the current model for SSA production from blowing snow showed that the parameterisations used can generally be applied to snow on sea ice. Snow salinity, a sensitive model parameter, depends to a first order on snowpack depth and therefore is higher above first-year than above multi-year sea ice. Shif

Blowing snow over sea ice has been proposed as a significant source of sea salt aerosol (SSA) (Yang et al., 2008). In this study, using snow salinity data and blowing snow and aerosol particle measurements collected in the Weddell Sea sea ice zone (SIZ) during a winter cruise, we perform a comprehensive model–data comparison with the aim of validating proposed parameterizations. Additionally, we investigate possible physical mechanisms involved in SSA production from blowing snow. A global chemical transport model, p-TOMCAT, is used to examine the model sensitivity to key parameters involved, namely blowing-snow size istribution, snow salinity, sublimation function, surface wind speed, relative humidity, air temperature and ratio of SSA formed per snow particle. As proposed in the parameterizations of Yang et al. (2008), the SSA mass flux is proportional to the bulk sublimation flux of blowing snow and snow salinity. To convert the bulk sublimation flux to SSA size distribution requires (1) sublimation function for snow particles, (2) blowing-snow size distribution, (3) snow (3) snow salinity and (4) ratio of SSA formed per snow particle. The optimum model–cruise aerosol data agreement (in diameter range of 0.4–12 μm) indicates two possible microphysical processes that could be associated with SSA production from blowing snow. The first one assumes that one SSA is formed per snow particle after sublimation, and snow particle sublimation is controlled by the curvature effect or the so-called “air ventilation” effect. The second mechanism allows multiple SSAs to form per snow particle and assumes snow particle sublimation is controlled by the moisture gradient between the surface of the particle and the ambient air (moisture diffusion effect). With this latter mechanism the model reproduces the observations assuming that one snow particle produces ~ 10 SSA during the sublimation process. Although both mechanisms generate very consistent results with respect to observe

The cryosphere, which comprises a large portion of Earth’s surface, is rapidly changing as a consequence of global climate change. Ice, snow, and frozen ground in the polar and alpine regions of the planet are known to directly impact atmospheric composition, which for example is observed in the large influence of ice and snow on polar boundary layer chemistry. Atmospheric inputs to the cryosphere, including aerosols, nutrients, and contaminants, are also changing in the anthropocene thus driving cryosphere-atmosphere feedbacks whose understanding is crucial for understanding future climate. Here, we present the Cryosphere and ATmospheric Chemistry initiative (CATCH) which is focused on developing new multidisciplinary research approaches studying interactions of chemistry, biology, and physics within the coupled cryosphere – atmosphere system and their sensitivity to environmental change. We identify four key science areas: (1) micro-scale processes in snow and ice, (2) the coupled cryosphere-atmosphere system, (3) cryospheric change and feedbacks, and (4) improved decisions and stakeholder engagement. To pursue these goals CATCH will foster an international, multidisciplinary research community, shed light on new research needs, support the acquisition of new knowledge, train the next generation of leading scientists, and establish interactions between the science community and society.

The cryosphere, which comprises a large portion of Earth’s surface, is rapidly changing as a consequence of global climate change. Ice, snow, and frozen ground in the polar and alpine regions of the planet are known to directly impact atmospheric composition, which for example is observed in the large influence of ice and snow on polar boundary layer chemistry. Atmospheric inputs to the cryosphere, including aerosols, nutrients, and contaminants, are also changing in the anthropocene thus driving cryosphere-atmosphere feedbacks whose understanding is crucial for understanding future climate. Here, we present the Cryosphere and ATmospheric Chemistry initiative (CATCH) which is focused on developing new multidisciplinary research approaches studying interactions of chemistry, biology, and physics within the coupled cryosphere – atmosphere system and their sensitivity to environmental change. We identify four key science areas: (1) micro-scale processes in snow and ice, (2) the coupled cryosphere-atmosphere system, (3) cryospheric change and feedbacks, and (4) improved decisions and stakeholder engagement. To pursue these goals CATCH will foster an international, multidisciplinary research community, shed light on new research needs, support the acquisition of new knowledge, train the next generation of leading scientists, and establish interactions between the science community and society

The Northern Hemisphere experienced dramatic changes during the last glacial, featuring vast ice sheets and abrupt climate events, while high northern latitudes during the last interglacial (Eemian) were warmer than today. Here we use high-resolution aerosol records from the Greenland NEEM ice core to reconstruct the environmental alterations in aerosol source regions accompanying these changes. Separating source and transport effects, we find strongly reduced terrestrial biogenic emissions during glacial times reflecting net loss of vegetated area in North America. Rapid climate changes during the glacial have little effect on terrestrial biogenic aerosol emissions. A strong increase in terrestrial dust emissions during the coldest intervals indicates higher aridity and dust storm activity in East Asian deserts. Glacial sea salt aerosol emissions in the North Atlantic region increase only moderately (50%), likely due to sea ice expansion. Lower aerosol concentrations in Eemian ice compared to the Holocene are mainly due to shortened atmospheric residence time, while emissions changed little.

Surface ozone has been measured since 2004 at the coastal East Antarctic site of Dumont d'Urville (DDU), and since 2007 at the Concordia station located on the high East Antarctic plateau. This paper discusses long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites. At Concordia, near-surface ozone data were complemented by balloon soundings and compared to similar measurements done at the South Pole. The DDU record is compared to those obtained at the coastal site of Syowa, also located in East Antarctica, as well as the coastal sites of Neumayer and Halley, both located on the coast of the Weddell Sea in West Antarctica. Surface ozone mixing ratios exhibit very similar seasonal cycles at Concordia and the South Pole. However, in summer the diurnal cycle of ozone is different at the two sites with a drop of ozone in the afternoon at Concordia but not at the South Pole. The vertical distribution of ozone above the snow surface also differs. When present, the ozone-rich layer located near the ground is better mixed and deeper at Concordia (up to 400 m) than at the South Pole during sunlight hours. These differences are related to different solar radiation and wind regimes encountered at these two inland sites. DDU appears to be the coastal site where the impact of the late winter/spring bromine chemistry is the weakest, but where the impact of elevated ozone levels caused by NOx snow emissions from the high Antarctic plateau is the highest. The highest impact of the bromine chemistry is seen at Halley and Neumayer, and to a lesser extent at Syowa. These three sites are only weakly impacted by the NOx chemistry and the net ozone production occurring on the high Antarctic plateau. The differences in late winter/spring are attributed to the abundance of sea ice offshore from the sites, whereas those in summer are related to the topography of East Antarctica that promotes the katabatic flow bri

A suite of 10 autonomous ozone monitoring units, each powered using renewable energy, was developed and built to study surface ozone in Antarctica during the International Polar Year (2007-2009). The monitoring systems were deployed in a network around the Weddell Sea sector of coastal Antarctica with a transect up onto the Antarctic Plateau. The aim was to measure for a full year, thus gaining a much-improved broader view of boundary layer ozone seasonality at different locations as well as of factors affecting the budget of surface ozone in Antarctica. Ozone mixing ratios were measured based on UV photometry using a modified version of the commercial 2B Technologies Inc. Model 202 instrument. All but one of the autonomous units measured successfully within its predefined duty cycle throughout the year, with some differences in performance dependent on power availability and ambient temperature. Mean data recovery after removal of outliers was on average 70% (range 44-83%) and precision varied between 1.5 and 8 ppbv, thus was sufficiently good to resolve year-round the main ozone features of scientific interest. We conclude that, with adequate power, and noting a minor communication problem, our units would be able to operate successfully at ambient temperatures down to -60 degrees C. Systems such as the one described in this paper, or derivatives of it, could therefore be deployed either as local or regional networks elsewhere in the Arctic or Antarctic. Here we present technical information and first results from the experiment.

Atmospheric hydroperoxides (ROOH) were measured at Summit, Greenland (72.97 degrees N, 38.77 degrees W) in summer 2003 (SUM03) and spring 2004 (SUM04) and South Pole in December 2003 (SP03). The two dominant hydroperoxides were H2O2 and CH3OOH (from here on MHP) with average (+/- 1 sigma) mixing ratios of 1448 (+/- 688) pptv, 204 (+/- 162) and 278 (+/- 67) for H2O2 and 578 (+/- 377) pptv, 139 (+/- 101) pptv and 138 (+/- 89) pptv for MHP, respectively. In early spring, MHP dominated the ROOH budget and showed night timemaxima and daytime minima, out of phase with the diurnal cycle of H2O2, suggesting that the organic peroxide is controlled by photochemistry, while H2O2 is largely influenced by temperature driven exchange between the atmosphere and snow. Highly constrained photochemical box model runs yielded median ratios between modeled and observed MHP of 52%, 148% and 3% for SUM03, SUM04 and SP03, respectively. At Summit firn air measurements and model calculations suggest a daytime sink of MHP in the upper snow pack, which decreases in strength through the spring season into the summer. Up to 50% of the estimated sink rates of 1-5 x 10(11) molecules m(-3) s(-1) equivalent to 24-96 pptv h(-1) can be explained by photolysis and reaction with the OH radical in firn air and in the quasi-liquid layer on snow grains. Rapid processing of MHP in surface snow is expected to contribute significantly to a photochemical snow pack source of formaldehyde (CH2O). Conversely, summer levels of MHP at South Pole are inconsistent with the prevailing high NO concentrations, and cannot be explained currently by known photochemical precursors or transport, thus suggesting a missing source. Simultaneous measurements of H2O2, MHP and CH2O allow to constrain the NO background today and potentially also in the past using ice cores, although it seems less likely that MHP is preserved in firn and ice.

An analysis of 96 snow pit and ice cores distributed over the Greenland ice sheet is used to determine the main drivers of variability in the preserved records of nitrate concentration. The data set provides samples from spatially distributed locations, allowing us to investigate the effect of snow accumulation rate, temperature, and sublimation on nitrate concentration. The mean ice sheet concentration in the dry snow zone (2000 >= mean annual sea level (masl)) is 132 ng g(-1), ranging between 47 and 265 ng g(-1) with a standard deviation of +/-37 ng g(-1). Nitrate flux varies between 1.1 and 14.7 mu g cm(-2) a(-1) with a mean of 4 +/- 2 mu g cm(-2) a(-1). Large-scale spatial variability exists as a result of accumulation gradients, with concentration 5% greater in the northern plateau, yet flux over the northern plateau is 30% lower than the dry snow zone as a whole. While spatially, flux appears to be more dependent on accumulation, preservation of flux shows increasing dependence on concentration with increasing accumulation. The relationship between concentration and accumulation is nonlinear, showing less dependence in the low-accumulation regions versus high-accumulation regions. Accumulation alone is insufficient to account for the observed variability in nitrate flux in the low-accumulation regions, and evidence supports the need for additional components to a transfer function model for nitrate that includes photochemistry, temperature, and sublimation. Spatial variability across the ice sheet is nonuniform, and changes in nitrate concentration have occurred in some regions at a greater rate than others. While the data support that overall the ice sheet acts as an archive of paleoatmospheric concentration despite the effects of postdepositional processing, one needs to consider spatial variables to properly account for trends and variability in the records. This is tested by evaluating past spatial relationships and yields the result that the significant g

The nitrogen (delta N-15) and triple oxygen (delta O-17 and delta O-18) isotopic composition of nitrate (NO3-) was measured year-round in the atmosphere and snow pits at Dome C, Antarctica (DC, 75.1 degrees S, 123.3 degrees E), and in surface snow on a transect between DC and the coast. Comparison to the isotopic signal in atmospheric NO3- shows that snow NO3- is significantly enriched in delta N-15 by > 200 parts per thousand and depleted in delta O-18 by < 40 parts per thousand. Post-depositional fractionation in delta O-17(NO3-) is small, potentially allowing reconstruction of past shifts in tropospheric oxidation pathways from ice cores. Assuming a Rayleigh-type process we find fractionation constants epsilon of -60 +/- 15 parts per thousand, 8 +/- 2 parts per thousand and 1 +/- 1 parts per thousand, for delta N-15, delta O-18 and delta O-17, respectively. A photolysis model yields an upper limit for the photolytic fractionation constant (15)epsilon of delta N-15, consistent with lab and field measurements, and demonstrates a high sensitivity of (15)epsilon to the incident actinic flux spectrum. The photolytic (15)epsilon is process-specific and therefore applies to any snow covered location. Previously published (15)epsilon values are not representative for conditions at the Earth surface, but apply only to the UV lamp used in the reported experiment (Blunier et al., 2005; Jacobi et al., 2006). Depletion of oxygen stable isotopes is attributed to photolysis followed by isotopic exchange with water and hydroxyl radicals. Conversely, N-15 enrichment of the NO3- fraction in the snow implies N-15 depletion of emissions. Indeed, delta N-15 in atmospheric NO3- shows a strong decrease from background levels (4 +/- 7 parts per thousand) to -35 parts per thousand in spring followed by recovery during summer, consistent with significant snowpack emissions of reactive nitrogen. Field and lab evidence therefore suggest that photolysis is an important process driving fracti

Satellite radar altimetry measurements indicate that the East Antarctic ice-sheet interior north of 81.6°S increased in mass by 45 ± 7 billion metric tons per year from 1992 to 2003. Comparisons with contemporaneous meteorological model snowfall estimates suggest that the gain in mass was associated with increased precipitation. A gain of this magnitude is enough to slow sea-level rise by 0.12 ± 0.02 millimeters per year.