Soot in the Arctic snowpack: a cause for perturbations in radiative transfer

Recent data collected in the Arctic have demonstrated the transport of atmospheric aerosol of anthropogenic origin into that region. Concern over the radiative effect of the highly-absorbing soot component of this aerosol has resulted in a variety of atmospheric sampling efforts aimed at assessing the climatic impact of this component. However, little attention has been given to the measurement of soot deposited on the Arctic snowpack and the resulting perturbation of snow albedo, snowmelt rates and radiative transfer. Here we report measurements of light-absorbing material in the Arctic snowpack for longitudes from 25 E to 160 W. The contributions to light absorption due to natural crustal and soot aerosol are identified by their wavelength dependence. Reductions in Arctic snow albedo of one to several percent appear probable for the soot/ice mass fractions obtained to date. Estimates of the impact of this reduced albedo on the Arctic radiation budget over a season are shown to approximately equal that of the Arctic haze itself. The absorption of shortwave radiation by the springtime snowpack is estimated to be 5–10 % higher than that of soot-free snow for this data.     

Total and methyl mercury patterns in Arctic snow during springtime at Resolute,Nunavut, Canada

Patterns of gaseous elemental mercury (GEM) were monitored at 20 and 150 cm above the snowpack near Resolute Bay, Cornwallis Island, Nunavut, Canada near the Upper Air Station of Environment Canada (74°42′N, 94°58′W) from 7 May (day 127) to 12 June (day 163) 2003. At this time of year there was 24 h daylight but still a strong diel change in solar radiation. Daily patterns of GEM-tracked solar radiation with a lag of about 2 h and the GEM gradient between these two heights showed the direction of flux. In addition to the previously established autocatalytic reactions involving halogens where reactive gaseous mercury and fine particulate mercury result in direct deposition to the snow, both diffusion to and volatilization from the snow occurred on a regular basis. Total mercury (THg) in the snowpack increased to near 30 ng L⁻¹ following 8 d of atmospheric mercury depletion then decreased to values near 1 ng L⁻¹. Losses from the snow could not be accounted for in melt water as stream runoff values were also low. In other words, most of the mercury associated with increased levels in snow was volatilized back to the atmosphere either directly from the snow or from the water surfaces. However, using accepted mass transport coefficients, the flux appeared low and other mechanisms are suggested. In contrast to THg, methyl mercury (MeHg) in the snow reached values near 140 pg L⁻¹ but also declined to less than detection limit (10 pg L⁻¹) with the onset of warmer temperatures. MeHg in stream runoff water was similar to maximal values seen in the snow. This observation is consistent with the view that MeHg came in the snowfall or was deposited to the snow pack rather than produced in the snow. In contrast, much of the THg associated with mercury depletion events was volatilized back to the atmosphere.     

On radiative effects of black carbon and sulphate aerosols

Most aerosol particles, such as sulphate and sea-salt particles, mainly scatter solar radiation, whilst soot (in the form of elemental carbon or “black” carbon, BC) in addition leads to considerable absorption. This scattering and absorption by the aerosol particles constitute the so-called direct aerosol effect. In this paper, we present results from a study of possible direct effects of tropospheric BC and sulphate aerosols, with an emphasis on BC aerosols, along a line from North Africa through Europe into the Arctic. Radiative budgets in a cloud-free atmosphere are estimated. Based on model-calculated distributions of BC and sulphate (provided by Seland and Iversen, 1998) and assumed size distributions of the background aerosol, new size distributions are obtained by adding natural, biomass burning and fossil fuel contributions to the background aerosol. Added nucleation mode particles are assumed externally mixed, whereas added accumulation mode BC and sulphate is internally mixed with the background according to condensational growth and Brownian coagulation theory. Humidity effects are taken into account by use of the Köhler equation. Mie calculations provide the resulting optical parameters, and the forcing is finally estimated by use of a radiative transfer model. A reference run and a series of eleven test-runs are performed to investigate the sensitivity of various assumptions on the contribution to upward TOA irradiance from BC and non-sea-salt sulphate. The tests suggest a high sensitivity to presence of BC and to particle swelling due to humidity. The sensitivity to assumed distribution of BC on particle size is more moderate. The same is true for the vertical resolution and the number concentration of the background aerosol. The effect of mixing organic carbon (OC) internally with biomass burning BC nucleation mode particles is characterized as moderate. The role of OC is, however, still uncertain. The same holds true for the optical thickness of the background atmosphere, for which we found a high sensitivity in this study. Other assumptions that were investigated had only small effects on the forcing. For the reference run we find a minimum in the aerosol forcing of approximately −5 W m^-2 near the most polluted areas in Europe, and a maximum of approximately 2 W m^-2 over North Africa. A warming effect is also found for the Arctic region, with forcing values up to 0.4 W m^-2.     

Direct radiative forcing and atmospheric absorption by boundary layer aerosols in the southeastern US: model estimates on the basis of new observations

In an effort to reduce uncertainties in the quantification of aerosol direct radiative forcing (ADRF) in the southeastern United States (US), a field column experiment was conducted to measure aerosol radiative properties and effects at Mt. Mitchell, North Carolina, and at an adjacent valley site. The experimental period was from June 1995 to mid-December 1995. The aerosol optical properties (single scattering albedo and asymmetry factor) needed to compute ADRF were obtained on the basis of a procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, aerosol optical depth, and diffuse-to-direct solar irradiance ratio. The regional values of ADRF at the surface and top of atmosphere (TOA), and atmospheric aerosol absorption are derived using the obtained aerosol optical properties as inputs to the column radiation model (CRM) of the community climate model (CCM3). The cloud-free instantaneous TOA ADRFs for highly polluted (HP), marine (M) and continental (C) air masses range from 20.3 to −24.8, 1.3 to −10.4, and 1.9 to −13.4 W m⁻², respectively. The mean cloud-free 24-h ADRFs at the TOA (at the surface) for HP, M, and C air masses are estimated to be −8±4 (−33±16), −7±4 (−13±8), and −0.14±0.05 (−8±3) W m⁻², respectively. On the assumption that the fractional coverage of clouds is 0.61, the annual mean ADRFs at the TOA and the surface are −2±1, and −7±2 W m⁻², respectively. This also implies that aerosols currently heat the atmosphere over the southeastern US by 5±3 W m⁻² on annual timescales due to the aerosol absorption in the troposphere.     

Regional climate forcing of aerosol estimated by a box model for a rural site in Central Europe during summer

In the present work, a box model is applied to estimate the direct climate forcing of aerosol particles for rural air in Central Europe during summertime. In the model, the input parameters reflect regional character: data from satellite observations and other surface measurements are used referring to the selected area, Hungary. In the calculation of direct climate forcing of aerosol particles satellite observations serve as the source of incoming solar radiation intensity data and cloudiness, while different aerosol parameters of the model (mass extinction coefficient, chemical composition, scale height, hygroscopic growth factor, etc.) are based on local measurements. Finally, surface albedo of the area studied was determined on the basis of vegetation cover and precipitation amount. As the summary of our calculations, in Central Europe direct climate forcing of ammonium sulfate is equal to –2.4 W m⁻². The climate forcing of total carbon is composed of two terms. The forcings due to scattering and absorption are –1.0 and +0.2 W m⁻², respectively. In spite of the fact that the mass concentrations of ammonium sulfate and total carbon are similar, their contribution to the aerosol direct forcing is different. We conclude that ammonium sulfate plays the major role in this process and organics have an additional impact.     

Platinum-group elements (Rh,Pt, Pd) and Au distribution in snow samples from the Kola Peninsula,NW Russia

In April 1996 snowpack samples were collected from the surroundings of the ore roasting and dressing plant at Zapoljarnij and the nickel smelters at Nikel and Monchegorsk, Kola Peninsula, NW Russia. In the laboratory, filter residues of snowpack samples (fraction>0.45 μm) from 15 localities (close to the nickel processing centres) were chemically for precious metals (Rh, Pt, Pd, Au) and Te by graphite furnace atomic absorption spectrometry (GFAAS) analysis, and for Cu and Ni by ICP-MS. Values up to 2770 ng/l Pd, 650 ng/l Pt and 186 ng/l Au were found in the filter residues. Additionally, platinum-group elements (PGE) and Au contents in ore samples from Noril’sk¹, as well as in technogenic products (“Cu–Ni-feinstein” and copper concentrate) processed at the Monchegorsk smelter complex, were analysed using flameless atomic absorption spectroscopy (FAAS) for comparison with results obtained from snow. Rh, Pt, Pd and Au distribution data show the presence of two ore components (Noril’sk and Pechenga). Concentrations of these metals decrease with distance from the industrial sources and with the prevailing wind direction (generally north–south). Microscopic investigations and electron microprobe analysis of polished sections of snow filter residues (>0.45 μm) also reveal differences between particles from the two sources.     

Snowpack processing of acetaldehyde and acetone in the Arctic atmospheric boundary layer

Acetaldehyde (CH₃CHO) and acetone (CH₃C(O)CH₃) concentrations in ambient air, in snowpack air, and bulk snow were determined at Alert, Nunavut, Canada, as a part of the Polar Sunrise Experiment (PSE): ALERT 2000. During the period of continuous sunlight, vertical profiles of ambient and snowpack air exhibited large concentration gradients through the top ∼10 cm of the snowpack, implying a flux of carbonyl compounds from the surface to the atmosphere. From vertical profile and eddy diffusivity measurements made simultaneously on 22 April, acetaldehyde and acetone fluxes of 4.2(±2.1)×10⁸ and 6.2(±4.2)×10⁸ molecules cm⁻² s⁻¹ were derived, respectively. For this day, the sources and sinks of CH₃CHO from gas phase chemistry were estimated. The result showed that the snowpack flux of CH₃CHO to the atmosphere was as large as the calculated CH₃CHO loss rate from known atmospheric gas phase reactions, and at least 40 times larger (in the surface layer) than the volumetric rate of acetaldehyde produced from the assumed main atmospheric gas phase reaction, i.e. reaction of ethane with hydroxyl radicals. In addition, acetaldehyde bulk snow phase measurements showed that acetaldehyde was produced in or on the snow phase, likely from a photochemical origin. The time series for the observed CH₃C(O)CH₃, ozone (O₃), and propane during PSE 1995, PSE 1998, and ALERT 2000 showed a consistent anti-correlation between acetone and O₃ and between acetone and propane. However, our data and model simulations showed that the acetone increase during ozone depletion events cannot be explained by gas phase chemistry involving propane oxidation. These results suggest that the snowpack is a significant source of acetaldehyde and acetone to the Arctic boundary layer.     

Modelling the behaviour of PAHs during atmospheric transport from the UK to the Arctic

Persistent organic pollutants (POPs) such as PAHs are subject to long-range atmospheric transport, which can result in the contamination of remote areas such as the Arctic. A simple model was developed to describe the removal processes of four PAHs; fluorene (FLU), phenanthrene (PHEN), fluoranthene (FLA) and benzo[a]pyrene (B[a]P) transported over a 5 day period from a source area over the UK to the Russian Arctic. The purpose of this model was to study processes affecting the PAHs within the atmosphere, rather than their interaction with the earth's surface. The components to the model included gas/particle partitioning, reaction with OH radicals and dry and wet deposition (both rain and snow). Atmospheric/meteorological parameters for the geographical region of interest were generated from three-dimensional atmospheric models. Air concentrations were prescribed in the source area with no additional PAH inputs along the transect, both winter and summer scenarios were modelled. Reaction with OH was a major removal mechanism for gas-phase FLU, PHEN and FLA, most notably in the temperate atmosphere. Wet deposition in the form of snow accounted for the majority of PAH loss in the winter, although the gas and particle scavenging ratios used in this model ranged over several orders of magnitude. Using a 5 day transport scenario in a `1-hop’ event, the model predicted that a primary emission of FLA and B[a]P to the atmosphere of the southern UK, would not reach the Russian Arctic at a distance of ∼3500 km, assuming a constant windspeed of 10 m s⁻¹. However, both FLU and PHEN with calculated half-lives of >60 h during the winter could be transported to this area under this scenario.     

On the contribution of black carbon to the composite aerosol radiative forcing over an urban environment

This paper discusses the extent of Black Carbon (BC) radiative forcing in the total aerosol atmospheric radiative forcing over Pune, an urban site in India. Collocated measurements of aerosol optical properties, chemical composition and BC were carried out for a period of six months (during October 2004 to May 2005) over the site. Observed aerosol chemical composition in terms of water soluble, insoluble and BC components were used in Optical Properties of Aerosols and Clouds (OPAC) to derive aerosol optical properties of composite aerosols. The BC fraction alone was used in OPAC to derive optical properties of BC aerosols. The aerosol optical properties for composite and BC aerosols were separately used in SBDART model to derive direct aerosol radiative forcing due to composite and BC aerosols. The atmospheric radiative forcing for composite aerosols were found to be +35.5, +32.9 and +47.6 Wm^?2 during post-monsoon, winter and pre-monsoon seasons, respectively. The average BC mass fraction found to be 4.83, 6.33 and 4 μg m^?3 during the above seasons contributing around 2.2 to 5.8% to the total aerosol load. The atmospheric radiative forcing estimated due to BC aerosols was +18.8, +23.4 and +17.2 Wm^?2, respectively during the above seasons. The study suggests that even though BC contributes only 2.2–6% to the total aerosol load; it is contributing an average of around 55% to the total lower atmospheric aerosol forcing due to strong radiative absorption, and thus enhancing greenhouse warming.     

Characterization of aerosol over the Northern South China Sea during two cruises in 2003

Atmospheric transport of trace elements has been found to be an important pathway for their input to the ocean. TSP, PM10, and PM2.5 aerosol samples were collected over the Northern South China Sea in two cruises in 2003 to estimate the input of aerosol from continent to the ocean. About 23 elements and 14 soluble ions in aerosol samples were measured. The average mass concentration of TSP in Cruise I in January (78 μg m⁻³) was ∼twice of that in Cruise II in April (37 μg m⁻³). Together with the crustal component, heavy metals from pollution sources over the land (especially from the industry and automobiles in Guangzhou) were transported to and deposited into the ocean. The atmospheric MSA concentrations in PM2.5 (0.048 μg m⁻³ in Cruise I and 0.043 μg m⁻³ in Cruise II) over Northern South China Sea were comparable to those over other coastal regions. The ratio of non-sea-salt (NSS)-sulfate to MSA is 103-655 for Cruise I and 15-440 for Cruise II in PM2.5 samples, which were much higher than those over remote oceans. The estimated anthropogenic sulfate accounts for 83–98% in Cruise I and 63–95% in Cruise II of the total NSS-sulfate. Fe (II) concentration in the aerosols collected over the ocean ranged from 0.1 to 0.9 μg m⁻³, accounting for 16–82% of the total iron in the aerosol, which could affect the marine biogeochemical cycle greatly.     

Variability in ultraviolet total optical depth during the Southern California Ozone Study (SCOS97)

Formation of photochemical air pollution is governed in part by the solar ultraviolet actinic radiation flux, but wavelength-resolved measurements of UV radiation in polluted urban atmospheres are rarely available. As part of the 1997 Southern California Ozone Study, cosine weighted solar irradiance was measured continuously at seven UV wavelengths (300, 306, 312, 318, 326, 333 and 368 nm) at two sites during the period 1 July to 1 November 1997. The first site was at Riverside (260 m a.s.l.) in the Los Angeles metropolitan area, which frequently experiences severe air pollution episodes. The second site was at Mt Wilson (1725 m a.s.l.), approximately 70 km northwest of Riverside, and located above much of the urban haze layer. Measurements of direct (i.e., total minus diffuse) solar irradiance were used to compute total atmospheric optical depths. At 300 nm, optical depths (mean±1 S.D.) measured over the entire study period were 4.3±0.3 at Riverside and 3.7±0.2 at Mt Wilson. Optical depth decreased with increasing wavelength, falling at 368 nm to values of 0.8±0.2 at Riverside and 0.5±0.1 at Mt Wilson. At all wavelengths, both the mean and the relative standard deviation of optical depths were larger at Riverside than at Mt Wilson. At 300 nm, the difference between the smallest and largest observed optical depths corresponds to over a factor 2 increase in the direct beam irradiance for overhead sun, and over a factor 7 increase for a solar zenith angle of 60°. Principal component analysis was used to reveal underlying factors contributing to variability in optical depths. PCA showed that a single factor (component) was responsible for the major part of the variability. At Riverside, the first component was responsible for 97% of the variability and the second component for 2%. At Mt Wilson, 89% of the variability could be attributed to the first component and 10% to the second. Dependence of the component contributions on wavelength allowed identification of probable physical causes: the first component is linked to light scattering and absorption by atmospheric aerosols, and the second component is linked to light absorption by ozone. These factors are expected to contribute to temporal and spatial variability in solar actinic flux and photodissociation rates of species including ozone, nitrogen dioxide, and formaldehyde.     

Pollution influences on atmospheric composition and chemistry at high northern latitudes: Boreal and California forest fire emissions

We analyze detailed atmospheric gas/aerosol composition data acquired during the 2008 NASA ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) airborne campaign performed at high northern latitudes in spring (ARCTAS-A) and summer (ARCTAS-B) and in California in summer (ARCTAS-CARB). Biomass burning influences were widespread throughout the ARCTAS campaign. MODIS data from 2000 to 2009 indicated that 2008 had the second largest fire counts over Siberia and a more normal Canadian boreal forest fire season. Near surface arctic air in spring contained strong anthropogenic signatures indicated by high sulfate. In both spring and summer most of the pollution plumes transported to the Arctic region were from Europe and Asia and were present in the mid to upper troposphere and contained a mix of forest fire and urban influences. The gas/aerosol composition of the high latitude troposphere was strongly perturbed at all altitudes in both spring and summer. The reactive nitrogen budget was balanced with PAN as the dominant component. Mean ozone concentrations in the high latitude troposphere were only minimally perturbed (<5 ppb), although many individual pollution plumes sampled in the mid to upper troposphere, and mixed with urban influences, contained elevated ozone (ΔO₃/ΔCO = 0.11 ± 0.09 v/v). Emission and optical characteristics of boreal and California wild fires were quantified and found to be broadly comparable. Greenhouse gas emission estimates derived from ARCTAS-CARB data for the South Coast Air Basin of California show good agreement with state inventories for CO₂ and N₂O but indicate substantially larger emissions of CH₄. Simulations by multiple models of transport and chemistry were found to be broadly consistent with observations with a tendency towards under prediction at high latitudes.     

Recent atmospheric Pb deposition at a rural site in southern Germany assessed using a peat core and snowpack,and comparison with other archives

In a peat bog from Black Forest, Southern Germany, the rate of atmospheric Pb accumulation was quantified using a peat core dated by ²¹⁰Pb and ¹⁴C. The most recent Pb accumulation rate (2.5 mg m⁻² y⁻¹) is similar to that obtained from a snowpack on the bog surface, which was sampled during the winter 2002 (1 to 4 mg m⁻² y⁻¹). The Pb accumulation rates recorded by the peat during the last 25 yr are also in agreement with published values of direct atmospheric fluxes in Black Forest. These values are 50 to 200 times greater than the “natural” average background rate of atmospheric Pb accumulation (20 μg m⁻² y⁻¹) obtained using peat samples from the same bog dating from 3300 to 1300 cal. yr B.C. The isotopic composition of Pb was measured in both the modern and ancient peat samples as well as in the snow samples, and clearly shows that recent inputs are dominated by anthropogenic Pb. The chronology and isotopic composition of atmospheric Pb accumulation recorded by the peat from the Black Forest is similar to the chronologies reported earlier using peat cores from various peat bogs as well as herbarium samples of Sphagnum and point to a common Pb source to the region for the past 150 years. In contrast, Pb contamination occurring before 1850 in southwestern Germany, differs from the record published for Switzerland mainly due to the mining activity in Black Forest. Taken together, the results show that peat cores from ombrotrophic bogs can yield accurate records of atmospheric Pb deposition, provided that the cores are carefully collected, handled, prepared, and analysed using appropriate methods.     

Spatial and seasonal variations of elemental composition in Mt. Everest (Qomolangma) snow/firn

In May 2005, a total of 14 surface snow (0–10 cm) samples were collected along the climbing route from the advanced base camp to the summit (6500–8844 m a.s.l.) on the northern slope of Mt. Everest (Qomolangma). A 108 m firn/ice core was retrieved from the col of the East Rongbuk Glacier (28.03°N, 86.96°E, 6518 m a.s.l.) on the north eastern saddle of Mt. Everest in September 2002. Surface snow and the upper 3.5 m firn samples from the core were analyzed for major and trace elements by inductively coupled plasma mass spectroscopy (ICP-MS). Measurements show that crustal elements dominated both surface snow and the firn core, suggesting that Everest snow chemistry is mainly influenced by crustal aerosols from local rock or prevalent spring dust storms over southern/central Asia.There are no clear trends for element variations with elevation due to local crustal aerosol inputs or redistribution of surface snow by strong winds during the spring. Seasonal variability in snow/firn elements show that high elemental concentrations occur during the non-monsoon season and low values during the monsoon season. Ca, Cr, Cs, and Sr display the most distinct seasonal variations. Elemental concentrations (especially for heavy metals) at Mt. Everest are comparable with polar sites, generally lower than in suburban areas, and far lower than in large cities. This indicates that anthropogenic activities and heavy metal pollution have little effect on the Mt. Everest atmospheric environment. Everest firn core REE concentrations are the first reported in the region and seem to be comparable with those measured in modern and Last Glacial Maximum snow/ice samples from Greenland and Antarctica, and with precipitation samples from Japan and the East China Sea. This suggests that REE concentrations measured at Everest are representative of the background atmospheric environment.     

Chemical composition of snowfall in the high Arctic: 1990–1994

From 1990 to 1994 at Alert, Nunavut, Canada, weekly snow samples were collected under low wind conditions to avoid contamination by blowing snow. They were analysed for major ions, Br⁻, and the organic ions methylsulphonate, formate, acetate and propionate. In the Arctic, where annual precipitation is low and blowing snow is common, these observations are unique. On an equivalent weight basis, acids and sea salt in snowfall are mixed approximately equally from December to January but from March to May acids dominate. The acidity of snowfall increases progressively throughout the winter to a May peak of ∼16 μeq l⁻¹. SO₄²⁻, Br⁻, and the organic acids acetate, and propionate peak in snowfall after polar sunrise indicate the influence of enhanced photochemical reactions. The greater enrichment of halides relative to sea salt Na⁺ in snow compared to aerosols indicates that gaseous uptake by snowflakes is important in the removal of these substances from the atmosphere and their deposition on to the Earth's surface. There is a marked difference between the seasonal variation of enrichment of Cl⁻ and Br⁻ in snow. The latter show a marked increase after polar sunrise while the former does not. These results provide valuable baseline information on the ionic content of fresh snowfall to be used in understanding the results of snowpack chemistry and post-depositional process studies conducted in the high Arctic.     

Size segregated water uptake of the urban submicrometer aerosol in Beijing

Physical and chemical properties of submicrometer aerosol particles were measured in summer 2004 (June/July) and winter 2005 (January/February) in Beijing, Peoples Republic of China, using a Twin-Differential Mobility Particle Sizer (T-DMPS), a Hygroscopicity-Tandem Differential Mobility Analyzer (H-TDMA), and a Micro Orifice Uniform Deposit Impactor (MOUDI). Particle number–size distributions were measured in the diameter range Dp = 3–800 nm and hygroscopic properties were determined at initial dry particle diameters of Dp_j (j = 30, 50, 80, 150, 250, and 350 nm) at a relative humidity (RH) of 90%. Hygroscopic properties were compared with chemical analyses of aerosol samples taken with the MOUDI. Based on the hygroscopicity data, the total hygroscopic particle volume was modeled, including dependence on dry particle size, season and level of pollution using a simple approach.Overall, the chemical analysis showed ammonium sulfate to be the major inorganic component of the urban submicrometer aerosol in Beijing along with relatively high fractions of elemental carbon (10–25%) and organic matter (15–60%) depending on particle size and season.The hygroscopic growth distributions (H-TDMA) subdivided the aerosol population into three different groups of particles with varying growth factors depending on dry particle size, namely nearly hydrophobic (growth factor = 0.96–1.07), less hygroscopic (1.06–1.29) and more hygroscopic (1.26–1.62).Hydrophobic particle fractions indicating freshly emitted soot/carbonaceous particles varied between 10 and 32% depending on dry particle size and season. During heavily polluted times, a decreasing number of hydrophobic particle fractions indicated that the urban submicrometer aerosol in Beijing was highly influenced by more aged aerosol transported from the industrial regions around Beijing containing sulfate as a major component.Based on model calculations, the urban submicrometer aerosol in Beijing showed strong compositional variations. The calculated total hygroscopic volume fractions varied between 16 and 65% depending on size, level of pollution and season.     

Ozone uptake to the polar snowpack at Summit,Greenland

The uptake of atmospheric ozone to the polar, year-round snowpack on glacial ice was studied at Summit, Greenland during three experiments in 2003, 2004, and 2005. Ozone was measured at up to three depths in the snowpack, on the surface, and above the surface at three heights on a tower along with supporting meteorological parameters. Ozone in interstitial air decreased with depth, albeit ozone gradients showed a high variation depending on environmental conditions of solar radiation and wind speed. Under low irradiance levels, up to 90% of ozone was preserved up to 1 m depth in the snowpack. Ozone depletion rates increased significantly with the seasonal and diurnal cycle of solar irradiance, resulting in only 10% of ozone remaining in the snowpack following solar noon during summertime. Faster snowpack air exchange from wind pumping resulted in smaller above-surface-to-within snowpack ozone gradients. These data indicate that the uptake of ozone to polar snowpack is strongly dependent on solar irradiance and wind pumping. Ozone deposition fluxes to the polar snowpack are consequently expected to follow incoming solar radiation levels and to exhibit diurnal and seasonal cycles. The Summit observations are in stark contrast to recent findings in the seasonal, midlatitude snowpack [Bocquet, F., Helmig, D., Oltmans, S.J., 2007. Ozone in the mid-latitude snowpack at Niwot Ridge, Colorado. Arctic, Antarctic and Alpine Research, in press], where mostly light-independent ozone behavior was observed. These contrasting results imply different ozone chemistry and snowpack–atmosphere gas exchange in the snow-covered polar, glacial conditions compared to the temperate, mid-latitude environment.     

Snow-to-air exchanges of mercury in an Arctic seasonal snow pack in Ny-Ålesund,Svalbard

The study of mercury (Hg) cycle in Arctic regions is a major subject of concern due to the dramatic increases of Hg concentrations in ecosystem in the last few decades. The causes of such increases are still in debate, and an important way to improve our knowledge on the subject is to study the exchanges of Hg between atmosphere and snow during springtime. We organized an international study from 10 April to 10 May 2003 in Ny-Ålesund, Svalbard, in order to assess these fluxes through measurements and derived calculations.Snow-to-air emission fluxes of Hg were measured using the flux chamber technique between ∼0 and 50 ng m⁻² h⁻¹. A peak in Gaseous Elemental Mercury (GEM) emission flux from the snow to the atmosphere has been measured just few hours after an Atmospheric Mercury Depletion Event (AMDE) recorded on 22 April 2004. Surprisingly, this peak in GEM emitted after this AMDE did not correspond to any increase in Hg concentration in snow surface. A peak in GEM flux after an AMDE was observed only for this single event but not for the four other AMDEs recorded during this spring period.In the snow pack which is seasonal and about 40 cm depth above permafrost, Hg is involved in both production and incorporation processes. The incorporation was evaluated to ∼5–40 pg m² h. Outside of AMDE periods, Hg flux from the snow surface to the atmosphere was the consequence of GEM production in the air of snow and was about ∼15–50 ng m⁻² h⁻¹, with a contribution of deeper snow layers evaluated to ∼0.3–6.5 ng m⁻² h⁻¹. The major part of GEM production is then mainly a surface phenomenon. The internal production of GEM was largely increasing when snow temperatures were close to melting, indicating a chemical process occurring in the quasi-liquid layer at the surface of snow grains.     

In-stack emissions of heavy metals estimated by moss biomonitoring method and snow-pack analysis

Data from the chemical analysis of moss growing close to a thermal power station and snowpack have been used for the estimation of heavy metal deposition close to the point pollution sources. A semi-empirical model was proposed to describe atmospheric trace metal deposition close to the point pollution source. Model parameters were derived from experimental data, and nickel and vanadium quantities, washed out with snow and rain, were calculated. Using long-term meteorological observation data of rain and snow duration and metal uptake efficiencies in moss, the average emission rates of vanadium and nickel from the stack were calculated. The coincidence between data from emission inventory and model results was within 25%. It was estimated that in the vicinity of pollution source (within 30 km) about 15% out of total emitted metals were washed out by rain and snow events. Metal concentrations in the environment become indistinguishable from the background at a distance of about 20 km from the stack.     

Measurements of JNO3− in snow by nitrate-based actinometry

Chemical actinometry was used to measure nitrate photolysis rate coefficients, J_NO3⁻, on and in snowpack at Summit, Greenland. Sealed glass tubes containing nitrate and a hydroxyl radical trapping system were buried in snow and exposed for between 2 and 24 h. Average J_NO3⁻ values for 2-h midday exposures in early June on surface snow were 10–14×10⁻⁷ s⁻¹. Averages over 24 h were 3.5–4.5×10⁻⁷ s⁻¹. These values reflect the integrated photon flux and also any variation of the nitrate photolysis rate with temperature. Attenuation of J_NO3⁻ within the firn was 0.03–0.04 cm⁻¹ for 24-h exposures and 0.08 cm⁻¹ for a 2-h exposure. Different attenuation coefficients may relate to differential light penetration due to changes in sun angle over the course of 24 h.