scholarly journals The origin of sea salt in snow on Arctic sea ice and in coastal regions

2004 ◽  
Vol 4 (9/10) ◽  
pp. 2259-2271 ◽  
Author(s):  
F. Domine ◽  
R. Sparapani ◽  
A. Ianniello ◽  
H. J. Beine

Abstract. Snow, through its trace constituents, can have a major impact on lower tropospheric chemistry, as evidenced by ozone depletion events (ODEs) in oceanic polar areas. These ODEs are caused by the chemistry of bromine compounds that originate from sea salt bromide. Bromide may be supplied to the snow surface by upward migration from sea ice, by frost flowers being wind-blown to the snow surface, or by wind-transported aerosol generated by sea spray. We investigate here the relative importance of these processes by analyzing ions in snow near Alert and Ny-Ålesund (Canadian and European high Arctic) in winter and spring. Vertical ionic profiles in the snowpack on sea ice are measured to test upward migration of sea salt ions and to seek evidence for ion fractionation processes. Time series of the ionic composition of surface snow layers are investigated to quantify wind-transported ions. Upward migration of unfractionated sea salt to heights of at least 17cm was observed in winter snow, leading to Cl- concentration of several hundred µM. Upward migration thus has the potential to supply ions to surface snow layers. Time series show that wind can deposit aerosols to the top few cm of the snow, leading also to Cl- concentrations of several hundred µM, so that both diffusion from sea ice and wind transport can significantly contribute ions to snow. At Ny-Ålesund, sea salt transported by wind was unfractionated, implying that it comes from sea spray rather than frost flowers. Estimations based on our results suggest that the marine snowpack contains about 10 times more Na+ than the frost flowers, so that both the marine snowpack and frost flowers need to be considered as sea salt sources. Our data suggest that ozone depletion chemistry can significantly enhance the Br- content of snow. We speculate that this can also take place in coastal regions and contribute to propagate ODEs inland. Finally, we stress the need to measure snow physical parameters such as permeability and specific surface area to understand quantitatively changes in snow chemistry.

2004 ◽  
Vol 4 (4) ◽  
pp. 4737-4776 ◽  
Author(s):  
F. Domine ◽  
R. Sparapani ◽  
A. Ianniello ◽  
H. J. Beine

Abstract. Snow, through its trace constituents, can have a major impact on lower tropospheric chemistry, as evidenced by ozone depletion events (ODEs) in oceanic polar areas. These ODEs are caused by the chemistry of bromine compounds, that originate from sea salt bromide. According to current ideas, bromide may be supplied to the snow surface either by upward migration from sea ice or by frost flowers being wind-blown to the snow surface. We investigate here the relative importance of both these processes by analyzing mineral ions in snow samples collected near Alert and Ny-Ålesund (Canadian and European high Arctic) in winter and spring. Vertical ionic profiles in the snowpack on sea ice are measured to test upward migration of sea salt ions and to seek evidence for ion fractionation processes. Time series of the ionic composition of surface snow layers are investigated to quantify wind-transported ions. Upward migration of unfractionated sea salt, to heights of at least 17 cm, was observed in snow sampled in winter, at temperatures near −30°C, leading to Cl− concentration of several hundred µM. Upward migration thus has the potential to supply ions to surface snow layers. Time series show that wind can deposit aerosols to the top few cm of the snow, leading also to Cl− concentrations of several hundred µM, so that both migration from sea ice and wind transport can significantly contribute ions to snow. At Ny-Ålesund, sea salt transported by wind was unfractionated, implying that it does not come from frost flowers. In the Arctic, frost flowers thus do not appear necessary to lead to large sea salt concentrations in surface snow, and to supply the bromide needed for ODEs. The data obtained also indicate that ODEs lead to significant deposition of Br− to snow. We speculate that this can also take place in coastal regions and contribute to propagate ODEs inland. Finally, we stress the need to measure snow physical parameters such as permeability and specific surface area, to understand quantitatively changes in snow chemistry.


2018 ◽  
Author(s):  
Jiayue Huang ◽  
Lyatt Jaeglé ◽  
Viral Shah

Abstract. Sea salt aerosols (SSA) produced on sea ice surfaces by blowing snow events or lifting of frost flower crystals have been suggested as important sources of SSA during winter over polar regions. The magnitude and relative contribution of blowing snow and frost flower SSA sources, however, remain uncertain. In this study, we use 2007–2009 aerosol extinction coefficients from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument onboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite and the GEOS-Chem global chemical transport model to constrain sources of SSA over Arctic and Antarctic sea ice. CALIOP retrievals show elevated levels of aerosol extinctions (10–20 Mm−1) in the lower troposphere (0–2 km) over polar regions during cold months. The standard GEOS-Chem model underestimates the CALIOP aerosol extinctions by 50–70 %. Adding frost flower emissions of SSA fails to explain the CALIOP observations. With blowing snow SSA emissions, the model captures the overall spatial and seasonal variation of CALIOP aerosol extinctions over the polar regions, but overestimates springtime aerosol extinctions over Arctic sea ice and winter-spring extinctions over Antarctic sea ice. We reduce the surface snow salinity over multi-year sea ice and infer the monthly FYI snow salinity required to minimize the discrepancy between CALIOP extinctions and the GEOS-Chem simulation. The empirically-derived snow salinity shows a decreasing trend in between fall and spring. The optimized blowing snow model with inferred snow salinities generally agrees with CALIOP extinction observations to within 10 % over sea ice, but underestimates aerosol extinctions over the regions where frost flowers are expected to have a large influence. Frost flowers could thus contribute indirectly to SSA production by increasing the local surface snow salinity and, therefore, the SSA production from blowing snow. We carry out a case study of an Arctic blowing snow SSA feature predicted by GEOS-Chem and sampled by CALIOP. Using backtrajectories, we link this feature to a blowing snow event which occurred 2 days earlier over first-year sea ice and was also detected by CALIOP.


2004 ◽  
Vol 39 ◽  
pp. 276-282 ◽  
Author(s):  
Andrew M. Rankin ◽  
Eric W. Wolff ◽  
Robert Mulvaney

AbstractIt has recently been shown that much sea-salt aerosol around the coast of Antarctica is generated not from open water, but from the surface of newly formed sea ice. Previous interpretations of ice-core records have disregarded the sea-ice surface as a source of sea salt. The majority of sea-salt aerosol at Halley research station originates from frost flowers rather than open water, and the seasonal cycle of sea salt in aerosol at Halley appears to be controlled by ice production in the Weddell Sea, as well as variations in wind speed. Frost flowers are also an important source of aerosol at Siple Dome, suggesting that variations in sea-salt concentrations in the core, and other cores drilled in similar locations, may be reflecting changes in sea-ice production rather than changes in transportation patterns. For Greenland cores, and those from low-accumulation inland sites in Antarctica, it is not simple to calculate the proportion of sea salt originating from frost flowers rather than open water. However, modelling studies suggest that a sea-ice surface source contributed much of the flux of sea salt to these sites in glacial periods, suggesting that interpretations of ice-core records from these locations should also be revisited.


2010 ◽  
Vol 22 (4) ◽  
pp. 435-441 ◽  
Author(s):  
M. Thamban ◽  
C.M. Laluraj ◽  
K. Mahalinganathan ◽  
B.L. Redkar ◽  
S.S. Naik ◽  
...  

AbstractSpatial variations in the ion composition were studied in 55 surface snow samples collected along three transects in the Ingrid Christensen Coast of East Antarctica. The sea-salt ion constituents revealed a drastic reduction from the ice edge to inland sites. The computed sea-salt sodium and non-sea-salt calcium concentrations suggest that while sea spray primarily contributes to the Na+, the crustal contribution dominates the Ca2+ in snow samples. The Cl-/ssNa+ ratios of the snow samples from the Larsemann transect varied between 4.7 and 1.05, indicating that additional Cl- sources like soil dust are important in the inland sites. The enrichment factors (Ef) confirm a dominant crustal source for Ca2+ in all transects. The Ef(K+) values indicate a dominant sea spray source for K+ in the coastal stations of the Larsemann and Publications transects. The Ef(Mg2+) values indicate the absence of any significant Mg2+ enrichment compared to seawater values. Secondary sulphur species (nssSO42- and MSA) within the snow samples suggest that both vary independently of each other, possibly influenced by the local biological activities. The nssSO42- data revealed that several summer snow deposits in the study region are significantly fractionated, apparently related to the sea ice existence during summer.


2011 ◽  
Vol 11 (8) ◽  
pp. 3949-3979 ◽  
Author(s):  
K. Toyota ◽  
J. C. McConnell ◽  
A. Lupu ◽  
L. Neary ◽  
C. A. McLinden ◽  
...  

Abstract. Episodes of high bromine levels and surface ozone depletion in the springtime Arctic are simulated by an online air-quality model, GEM-AQ, with gas-phase and heterogeneous reactions of inorganic bromine species and a simple scheme of air-snowpack chemical interactions implemented for this study. Snowpack on sea ice is assumed to be the only source of bromine to the atmosphere and to be capable of converting relatively stable bromine species to photolabile Br2 via air-snowpack interactions. A set of sensitivity model runs are performed for April 2001 at a horizontal resolution of approximately 100 km×100 km in the Arctic, to provide insights into the effects of temperature and the age (first-year, FY, versus multi-year, MY) of sea ice on the release of reactive bromine to the atmosphere. The model simulations capture much of the temporal variations in surface ozone mixing ratios as observed at stations in the high Arctic and the synoptic-scale evolution of areas with enhanced BrO column amount ("BrO clouds") as estimated from satellite observations. The simulated "BrO clouds" are in modestly better agreement with the satellite measurements when the FY sea ice is assumed to be more efficient at releasing reactive bromine to the atmosphere than on the MY sea ice. Surface ozone data from coastal stations used in this study are not sufficient to evaluate unambiguously the difference between the FY sea ice and the MY sea ice as a source of bromine. The results strongly suggest that reactive bromine is released ubiquitously from the snow on the sea ice during the Arctic spring while the timing and location of the bromine release are largely controlled by meteorological factors. It appears that a rapid advection and an enhanced turbulent diffusion associated with strong boundary-layer winds drive transport and dispersion of ozone to the near-surface air over the sea ice, increasing the oxidation rate of bromide (Br−) in the surface snow. Also, if indeed the surface snowpack does supply most of the reactive bromine in the Arctic boundary layer, it appears to be capable of releasing reactive bromine at temperatures as high as −10 °C, particularly on the sea ice in the central and eastern Arctic Ocean. Dynamically-induced BrO column variability in the lowermost stratosphere appears to interfere with the use of satellite BrO column measurements for interpreting BrO variability in the lower troposphere but probably not to the extent of totally obscuring "BrO clouds" that originate from the surface snow/ice source of bromine in the high Arctic. A budget analysis of the simulated air-surface exchange of bromine compounds suggests that a "bromine explosion" occurs in the interstitial air of the snowpack and/or is accelerated by heterogeneous reactions on the surface of wind-blown snow in ambient air, both of which are not represented explicitly in our simple model but could have been approximated by a parameter adjustment for the yield of Br2 from the trigger.


2020 ◽  
Vol 20 (12) ◽  
pp. 7335-7358 ◽  
Author(s):  
Jiayue Huang ◽  
Lyatt Jaeglé ◽  
Qianjie Chen ◽  
Becky Alexander ◽  
Tomás Sherwen ◽  
...  

Abstract. We use the GEOS-Chem chemical transport model to examine the influence of bromine release from blowing-snow sea salt aerosol (SSA) on springtime bromine activation and O3 depletion events (ODEs) in the Arctic lower troposphere. We evaluate our simulation against observations of tropospheric BrO vertical column densities (VCDtropo) from the GOME-2 (second Global Ozone Monitoring Experiment) and Ozone Monitoring Instrument (OMI) spaceborne instruments for 3 years (2007–2009), as well as against surface observations of O3. We conduct a simulation with blowing-snow SSA emissions from first-year sea ice (FYI; with a surface snow salinity of 0.1 psu) and multi-year sea ice (MYI; with a surface snow salinity of 0.05 psu), assuming a factor of 5 bromide enrichment of surface snow relative to seawater. This simulation captures the magnitude of observed March–April GOME-2 and OMI VCDtropo to within 17 %, as well as their spatiotemporal variability (r=0.76–0.85). Many of the large-scale bromine explosions are successfully reproduced, with the exception of events in May, which are absent or systematically underpredicted in the model. If we assume a lower salinity on MYI (0.01 psu), some of the bromine explosions events observed over MYI are not captured, suggesting that blowing snow over MYI is an important source of bromine activation. We find that the modeled atmospheric deposition onto snow-covered sea ice becomes highly enriched in bromide, increasing from enrichment factors of ∼5 in September–February to 10–60 in May, consistent with composition observations of freshly fallen snow. We propose that this progressive enrichment in deposition could enable blowing-snow-induced halogen activation to propagate into May and might explain our late-spring underestimate in VCDtropo. We estimate that the atmospheric deposition of SSA could increase snow salinity by up to 0.04 psu between February and April, which could be an important source of salinity for surface snow on MYI as well as FYI covered by deep snowpack. Inclusion of halogen release from blowing-snow SSA in our simulations decreases monthly mean Arctic surface O3 by 4–8 ppbv (15 %–30 %) in March and 8–14 ppbv (30 %–40 %) in April. We reproduce a transport event of depleted O3 Arctic air down to 40∘ N observed at many sub-Arctic surface sites in early April 2007. While our simulation captures 25 %–40 % of the ODEs observed at coastal Arctic surface sites, it underestimates the magnitude of many of these events and entirely misses 60 %–75 % of ODEs. This difficulty in reproducing observed surface ODEs could be related to the coarse horizontal resolution of the model, the known biases in simulating Arctic boundary layer exchange processes, the lack of detailed chlorine chemistry, and/or the fact that we did not include direct halogen activation by snowpack chemistry.


2016 ◽  
Author(s):  
Keiichiro Hara ◽  
Sumito Matoba ◽  
Motohiro Hirabayashi ◽  
Tetsuhide Yamasaki

Abstract. Sea-salts and halogens in aerosols, frost flowers and brine play an important role in atmospheric chemistry in polar regions. Simultaneous sampling and observations of frost flowers, brine, and aerosol particles were conducted around Siorapaluk in north-western Greenland during December 2013–March 2014. Results show that water-soluble frost flower and brine constituents were sea salts (e.g., Na+, Cl−, Mg2+, and Br−). Concentration factors of sea-salt constituents of frost flowers and brine relative to seawater were 1.14–3.67. Sea-salt enrichments of Mg2+, K+, Ca2+, and halogens (Cl−, Br−, and I) in frost flowers were associated with sea-salt fractionation by precipitation of mirabilite and hydrohalite. Aerosol number concentrations, particularly in coarse mode, were increased considerably by release from the sea-ice surface under strong wind conditions. Sulphate depletion by sea-salt fractionation was found to be slight in sea-salt aerosols because of heterogeneous SO42− formation on sea-salt particles. However, coarse and fine sea-salt particles were found to be rich in Mg. Strong Mg enrichment might be more likely to proceed in fine sea-salt particles. Mg-rich sea-salt particles might be released from the sea-ice surface and frost flowers. Mirabilite-like and ikaite-like particles were identified only in aerosol samples collected near new sea-ice areas.


2017 ◽  
Vol 17 (13) ◽  
pp. 8577-8598 ◽  
Author(s):  
Keiichiro Hara ◽  
Sumito Matoba ◽  
Motohiro Hirabayashi ◽  
Tetsuhide Yamasaki

Abstract. Sea salts and halogens in aerosols, frost flowers, and brine play an important role in atmospheric chemistry in polar regions. Simultaneous sampling and observations of frost flowers, brine, and aerosol particles were conducted around Siorapaluk in northwestern Greenland during December 2013 to March 2014. Results show that water-soluble frost flower and brine components are sea-salt components (e.g., Na+, Cl−, Mg2+, K+, Ca2+, Br−, and iodine). Concentration factors of sea-salt components of frost flowers and brine relative to seawater were 1.14–3.67. Sea-salt enrichment of Mg2+, K+, Ca2+, and halogens (Cl−, Br−, and iodine) in frost flowers is associated with sea-salt fractionation by precipitation of mirabilite and hydrohalite. High aerosol number concentrations correspond to the occurrence of higher abundance of sea-salt particles in both coarse and fine modes, and blowing snow and strong winds. Aerosol number concentrations, particularly in coarse mode, are increased considerably by release from the sea-ice surface under strong wind conditions. Sulfate depletion by sea-salt fractionation was found to be limited in sea-salt aerosols because of the presence of non-sea-salt (NSS) SO42−. However, coarse and fine sea-salt particles were found to be rich in Mg. Strong Mg enrichment might be more likely to proceed in fine sea-salt particles. Magnesium-rich sea-salt particles might be released from the surface of snow and slush layer (brine) on sea ice and frost flowers. Mirabilite-like and ikaite-like particles were identified only in aerosol samples collected near new sea-ice areas. From the field evidence and results from earlier studies, we propose and describe sea-salt cycles in seasonal sea-ice areas.


2020 ◽  
Author(s):  
Jiayue Huang ◽  
Lyatt Jaeglé ◽  
Qianjie Chen ◽  
Becky Alexander ◽  
Tomás Sherwen ◽  
...  

Abstract. We use the GEOS-Chem chemical transport model to examine the influence of bromine release from blowing snow sea salt aerosol (SSA) on springtime bromine activation and O3 depletion events (ODEs) in the Arctic lower troposphere. We evaluate our simulation against observations of tropospheric BrO vertical column densities (VCDtropo) from the GOME-2 and OMI spaceborne instruments for three years (2007–2009), as well as against surface observations of O3. We conduct a simulation with blowing snow SSA emissions from first-year sea ice (FYI, with a surface snow salinity of 0.1 psu) and multi-year sea ice (MYI, with a surface snow salinity of 0.05 psu), assuming a factor of 5 bromide enrichment of surface snow relative to seawater. This simulation captures the magnitude of observed March–April GOME-2 and OMI VCDtropo to within 17 %, as well as their spatiotemporal variability (r = 0.76-0.85). Many of the large-scale bromine explosions are successfully reproduced, with the exception of events in May, which are absent or systematically underpredicted in the model. If we assume a lower salinity on MYI (0.01 psu) some of the bromine explosions events observed over MYI are not captured, suggesting that blowing snow over MYI is an important source of bromine activation. We find that the modeled atmospheric deposition onto snow-covered sea ice becomes highly enriched in bromide, increasing from enrichment factors of ~ 5 in September–February to 10–60 in May, consistent with freshly fallen snow composition observations. We propose that this progressive enrichment in deposition could enable blowing snow-induced halogen activation to propagate into May and might explain our late-spring underestimate in VCDtropo. We estimate that atmospheric deposition of SSA could increase snow salinity by up to 0.04 psu between February and April, which could be an important source of salinity for surface snow on MYI as well as FYI covered by deep snowpack. Inclusion of halogen release from blowing snow SSA in our simulations decreases monthly mean Arctic surface O3 by 4–8 ppbv (15–30 %) in March and 8–14 ppbv (30–40 %) in April. We reproduce a transport event of depleted O3 Arctic air down to 40º N observed at many sub-Arctic surface sites in early April 2007. While our simulation captures a few ODEs observed at coastal Arctic surface sites, it underestimates the magnitude of other events and entirely misses some events. We suggest that inclusion of direct snowpack activation, which is a strong local source of Br radicals in the shallow Arctic boundary layer, could help reconcile the success of our simulation at capturing satellite retrievals of VCDtropo with its difficulty in reproducing local ODEs.


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