Atmospheric transport and deposition of trace elements onto the Greenland Ice Sheet

Airborne particles of diameter > 0.4 μm reaching Dye 3, Greenland during April–May 1983 were highly variable in size and concentration from day to day. Five-day backward air mass trajectories suggest the importance of long-range transport from more northerly latitudes on days with high concentrations; particle sizes were larger on these days. Lower concentrations and smaller particle sizes were associated with transport from the south. It is inferred that Dye 3 may receive material emitted from Eurasian sources and transported over the Pole, similar to inferences for more northern Arctic sites.Elemental analysis of individual particles showed an abundance of crustal material, with many particles also containing sulfur. Bulk chemical analyses of airborne particles and fresh snow, collected during three snowstorms where ice nucleation dominated, provided data which were used to estimate mass-basis scavenging ratios. Average scavenging ratios were in the range ~1000–2000 for the crustal elements Al, Fe, K, Mg, Mn, and Na. Similar values were observed for Cd, Cu and NO₃⁻. The corresponding ratios for Pb and SO₄²⁻ averaged less than 200. These ratios were used with precipitation rate data to estimate wet deposition velocities in the order of ~2 cm s⁻¹ for the first nine species, and ~0.2 cm s⁻¹ for Pb and SO₄²⁻. Comparing fresh and older surface snow concentrations gave an average dry deposition velocity of roughly 0.2 cm s⁻¹ for the crustal elements, with the small fraction of large particles (~5–10 μm) dominating deposition; much smaller values were associated with the remaining species. When used with other data in the literature, the results of this study suggest that total deposition velocities of Pb and SO₄²⁻ may be as small as 0.05 cm s⁻¹ in relatively dry regions of the Arctic.     

Seasonal and spatial trends in south Greenland snow chemistry

The spatial, temporal, source and physical controls on chloride, nitrate, sulfate and sodium in south Greenland snow are presented in this paper based on chemical data from snowpit and fresh snow samples. The snowpit samples cover the period June 1982–June 1984 and the fresh surface snow samples represent one storm event sampled over a 38-km traverse from Dye 3 to the southwest. Oxygen isotope dated records of chloride, sodium, excess sulfate and nitrate are discussed with respect to input timing and source. Notably the anthropogenic influx of excess sulfate is apparent in addition to an influx of excess sulfate that coincides with and is attributed to the arrival of the El Chichon cloud in S Greenland. The El Chichon event is also marked by highs in chloride and nitrate. Examination of fresh surface snow reveals geographic, temperature and moisture controls on deposition. Some excess sulfate close to Dye 3 can be attributed to local pollution.     

Distinguishing the relative contribution of fossil fuel and biomass combustion aerosols deposited at Summit,Greenland through isotopic and molecular characterization of insoluble carbon

Quantifying combustion aerosols transported to Summit, Greenland has typically involved the measurement of water-soluble inorganic and organic ions in air, snow, and ice. However, the ubiquitous nature of atmospheric soluble ions makes it difficult to separate the combustion component from the natural component. More specific combustion indicators are therefore needed to accurately quantify inputs from biomass and fossil-fuel burning. This work reports on radiocarbon (¹⁴C) analysis of elemental carbon (EC) and quantification of polycyclic aromatic hydrocarbons (PAHs) of water-insoluble particles from a snowpit excavated at Summit, Greenland in 1996. The ¹⁴C measurements allowed us to quantify the relative contribution of EC from biomass burning and fossil-fuel combustion transported to and deposited at Summit during periods of 1994 and 1995. Specific PAHs associated with conifer combustion helped to identify snowpit layers impacted by forest fires. Our results show that fossil EC was the major component during spring and fall 1994, while biomass EC and fossil EC were present in roughly equal amounts during summer 1994. PAH ratios in spring layers of the snowpit indicate substantial inputs from anthropogenic sources and the ΣPAH depth profile displays springtime maxima that coincided with non-sea-salt sulfate ion maximum concentrations. In other layers, ammonium ion concentrations were independent of the isotopic and molecular carbon measurements. This work demonstrates the utility of radiocarbon techniques to quantify the two different sources of combustion-generated particles at Summit; however, portions of the ¹⁴C results were indeterminate due to large uncertainties that were the result of chemical impurities introduced in the EC isolation technique. Additionally, PAH measurements were successfully performed on as little as 100 ml of snowmelt water, demonstrating the potential for future finer sample resolution.     

A 100 year record of ion chemistry from Agassiz Ice Cap Northern Ellesmere Island NWT,Canada

Two ice cores from the top of Agassiz Ice Cap, one from a snow scoured and the other from an unscoured zone, cover 80 and 100 yr of snow deposition respectively. The time scale for the cores is based on seasonal ion signals, a known stratigraphic horizon (1962), and a marked volcanic signature of high SO^2-₄, representing Katmai (1912). A marked increase in the SO^2-₄ and NO^-₃ ion which began in the middle of the 19th century is compared with the earlier increase in Greenland and attributed to a different combination of aerosol sources. A case is made for dry deposition of ions in winter, based on the continued presence of winter ion peaks at a site that δ¹⁸O indicates has almost no winter snow accumulation. This case is supported by the snowfall record at a nearby Automatic Weather Station, which shows there is very little winter snowfall at these sites, and by the fact that different accumulation rates and ion concentrations at each site effect almost the same ion fluxes. There is no evidence in either of the cores for a change in the levels of pollutant NO^-₃ and SO^2-₄ ion concentrations, due to improvement in emission technologies in the western nations, over the last two decades. The lack of change may indicate that Russia is the dominant source for aerosols at this site.     

Wet and dry deposition monitoring in Southeastern Michigan

Wet and dry deposition as collected by a bucket were measured at two sites in southeastern Michigan for two years. The precipitation had an average pH of 4.27 and a SO²⁻₄ to NO⁻₃ ratio of 2.0. Particulate dry deposition velocities of 0.6 cm s⁻¹ for SO²⁻₄ and NO⁻₃ and > 2 cm s⁻¹ for Cl⁻, Ca²⁺, Mg²⁺,Na⁺ and K⁺ were calculated. The ambient particle composition, dry bucket collection and wet deposition were compared at two sites, one urban and the other rural. Higher ambient particle concentrations and dry deposition rates were measured at the urban site than the rural site, indicating the influence of local emissions. However, local emissions had no effect on the wet deposition concentrations. The influence of more distant source regions was examined by separating the precipitation events by wind direction. The events from the south and east had the highest SO²⁻₄ to NO⁻₃ ratios, which corresponded to the areas with the highest sulfur emissions. NO⁻₃ showed no directional dependence.Wet deposition was examined for the effect of storm type and seasonal trends. Contrary to a recent study on Long Island, we found higher concentrations of H⁺, SO²⁻₄ and NH⁺₄ in winter rain compared to snow. The wet deposition concentrations of H⁺, SO²⁻₄, and NH⁺₄ were highest in the summer, while only Na⁺ and Cl⁻ concentrations were highest in the winter, presumably due to winter road salting. The total deposition of acidic ions was highest in the summer and lowest in the winter, due both to lower concentrations and lower precipitation volumes in the winter. The dry deposition as collected by a bucket accounted for 1 % of total H⁺ deposition, 21 % of SO²⁻₄ deposition, 27% of NO⁻₃ deposition, 50% of Cl⁻ deposition and 61 % of Ca²⁺ deposition.     

An experimental study of the dry deposition of gaseous nitric acid to snow

A chamber placed in a constant temperature freezing room was used to study the surface resistance during deposition of HNO₃ to a snow surface. The resistance decreased with increasing temperature from larger than 5 s mm⁻¹ at − 18°C to about l s mm⁻¹ at −3°C. Measurements of gaseous and particulate nitrate concentrations during winter at a rural site in south central Sweden gave concentrations in the range of 0.4–5 μg HNO₃ m⁻¹ and 0.3–3 μg NO⁻₃ m⁻³ with a mean value of 1.3 μg HNO₃ m⁻³ and 0.7 μg NO⁻₃ m⁻³, respectively. The results indicate that for periods with temperatures below − 2°C estimated dry deposition of HNO₃ to snow is at most 4 % of measured wet deposition of nitrate in the area.     

Fast nitrogen oxide photochemistry in Summit,Greenland snow

During the 1999 summer field season at Summit, Greenland, we conducted several series of experiments to follow up on our 1998 discovery that NO_x is released from the sunlit snowpack. The 1999 experiments included measurements of HONO in addition to NO and NO₂, and were designed to confirm, for Greenland snow, that the processes producing reactive nitrogen oxides in the snow are largely photochemical. Long duration experiments (up to 48 h) in a flow-through chamber and in the natural snowpack revealed sun-synchronous diurnal variations of all three reactive nitrogen oxides. In a second set of experiments we alternately shaded or exposed snow (again in the natural snowpack and in the chamber) to ambient sunlight for short periods to reduce any temperature changes during variations in light intensity. All three N oxides increased (decreased) very rapidly when sunlit (shaded). In all experiments NO₂ was approximately 3-fold more abundant than NO and HONO (which were at similar levels). Higher concentrations of NO₃⁻ in the snow resulted in higher mixing ratios of HONO, NO and NO₂ in the snow pore air, consistent with our hypothesis that photolysis of NO₃⁻ is the source of the reactive N oxides.     

Long-term measurements of SO2 dry deposition over Gansu Province,China

Potassium carbonate sulfation plates, monitored monthly for 11 years from 48 sites in 11 cities in Gansu Province, China, provide a crude estimate of cumulative SO₂ dry depositions. Measured SO₂ dry deposition rates were 1.6–472 mg m⁻² day⁻¹ and had seasonal variations with maxima in winter and minima mainly during summer as a result of higher winter and lower summer SO₂ concentrations. The 11-year monthly average SO₂ dry deposition rates are 23.2–248.97 and 11.7–175.6 mg m⁻² day⁻¹ in the eleven cities in winter and summer, respectively. A monthly average SO₂ deposition velocity was also estimated from 0.06 to 9.72 cm s⁻² in the 11 cities studied with a 11-year average maximum value of about 1.1–2.7 cm s⁻² in April and July and a 11-year average minimum value of about 0.2–1.0 cm s⁻¹ in January. The SO₂ dry deposition velocity also exhibits an increasing with wind speed in basins of less than 500 mm annual precipitation. In contrast, due to influences of the relative humidity in valleys of more than 500 mm annual precipitation, it shows a decreasing trend with wind speed increasing.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Major ions and scavenging of sulphate in the norwegian arctic

Precipitation samples at eight sites in the Norwegian Arctic and Northern Norway have been collected and analyzed for the period June 1982–June 1984. The results are compared with data for airborne SO²⁻₄ and SO₂ measured at ground level, and information on concentrations at higher levels from aircraft measurements and model calculations.The scavenging coefficients are generally low under Arctic winter conditions, and high during summer. This can be explained by the different vertical distributions of scavenged material in summer and winter, and differences in precipitation-forming processes. In addition, local climatic conditions with high relative humidity and high concentrations of sea-spray particles result in locally enhanced scavenging efficiencies at the island stations Bjørnøya and Jan Mayen. High NH⁺₄ concentrations in precipitation occur near bird colonies during the breeding period.The wet deposition in the Arctic is small, i.e. an order of magnitude lower than in Southern Norway.     

Monitoring Deposition of Nitrogen-Containing Compounds in a High-Elevation Forest Canopy

Measurements of airborne (gaseous and aerosol), cloud water, and precipitation concentrations of nitrogen compounds were made at Mt. Mitchell State Park (Mt. Gibbs, ~2006 m MSL), North Carolina, during May through September of 1988 and 1989, An annular denuder system was used to ascertain gaseous (nitric acid, nitrous acid, and ammonia) and particulate (nitrate and ammonium) nitrogen species, and a chemiluminescence nitrogen oxides analyzer was used to measure nitric oxide and nitrogen dioxide. Measurements of NO₃ ^? and NH₄ ⁺ ions in cloud and rain water samples were made during the same time period. Mean concentrations of gaseous nitric acid, nitrous acid, and ammonia were 1.14 μg/m³, 0.3 μg/m³, and 0.62 μg/m³ for 1988, and 1.40 μg/m³,0.3 μg/m³, and 1.47 μg/m³ for 1989, respectively. Fine particulate nitrate and ammonium ranged from 0.02 to 0.21 μg/m³ and 0.01 to 4.72 μg/m³ for 1988, and 0.1 to 0.78 μg/m³ and 0.24 to 2.32 μg/m³ for 1989, respectively. The fine aerosol fraction was dominated by ammonium sulfate particles. Mean concentrations of nitrate and ammonium ions in cloud water samples were 238 and 214 μmol/l in 1988, and 135 and 147 μmol/l in 1989, respectively. Similarly, the concentrations of NO₃ and NH₄ ⁺ in precipitation were 26.4 and 14.0 μmol/l in 1988, and 16.6 and 15.2 μmol/l in 1989, respectively. The mean total nitrogen deposition due to wet, dry, and cloud deposition processes was estimated as ~30 and ~40 kg N/ha/year (i.e., ~10 and ~13 kg N/ha/growing season) for 1988 and 1989. Based on an analytical analysis, deposition to the forest canopy due to cloud interception, precipitation, and dry deposition processes was found to contribute ~60, ~20, and ~20 percent, respectively, of the total nitrogen deposition.     

Processes affecting the movement of organochlorine pesticides (OCPs) between soil and air in an industrial site in Turkey

Soil and atmospheric concentrations, dry deposition and soil-air gas exchange of organochlorine pesticides (OCPs) were investigated at an industrial site in Aliaga, Izmir, Turkey. Current-use pesticides, endosulfan and chlorpyrifos, had the highest atmospheric levels in summer and winter. Summertime total (gas + particle) OCP concentrations in air were higher, probably due to increased volatilization at higher temperatures and seasonal local/regional applications of current-use pesticides. Particle deposition fluxes were generally higher in summer than in winter. Overall average dry particle deposition velocity for all the OCPs was 4.9 ± 4.1 cm s⁻¹ (average ± SD). ΣDDXs (sum of p,p′-DDT, p,p′-DDD, and p,p′-DDE) were the most abundant OCPs in Aliaga soils (n = 48), probably due to their heavy historical use and persistence. Calculated fugacity ratios and average net gas fluxes across the soil-air interface indicated volatilization for α-CHL, γ-CHL, heptachlorepoxide, cis-nonachlor, trans-nonachlor, and p,p′-DDT in summer, and for α-CHL, γ-CHL, trans-nonachlor, endosulfan sulfate, and p,p′-DDT in winter. For the remaining OCPs, soil acted as a sink during both seasons. Comparison of the determined fluxes showed that dry particle, gas-phase, and wet deposition are significant OCP input mechanisms to the soil in the study area.     

Washout ratios of nitrate,non-sea-salt sulfate and sea-salt on Virginia key,Florida and on American Samoa

On Virginia Key, Miami, Florida, 257 rainwater samples were collected on a event basis from May 1982 to April 1985. At the same site, 171 aerosol samples were collected throughout 1984. All of these samples were analyzed for nitrate, non-sea-salt (NSS) sulfate and sodium to assess the temporal variations in the concentrations and to determine the washout ratios of each of the constituents. The annual volume-weighted mean concentrations in rainwater are: nitrate—0.51 μg ml⁻¹; NSS sulfate—0.74 μg ml⁻¹; Na—1.93 μg ml⁻¹. Only sodium exhibited a significant seasonal cycle; its concentrations were markedly higher during the winter. In aerosols, the mean concentrations are: nitrate—1.9 μg m⁻³; NSS sulfate—2.8 μg m³; Na—3.7 μg m⁻³. Nitrate and NSS sulfate exhibit consistent seasonal cycles with concentrations being significantly higher during the winter and spring. We estimate that wet deposition accounts for the majority of the total fluxes of each constituent: 80% for nitrate, 95 % for NSS sulfate, and 67% for Na. Annual washout ratios at Virginia Key arc similar for nitrate and NSS sulfate, 330 and 290, respectively. That for Na is about a factor of two higher, 550. Comparable long-term ratios were calculated for American Samoa based on aerosol data from the SEAREX program and rainwater data from the National Atmospheric Deposition Program: 270 for nitrate, 420 for NSS sulfate, and 520 for Na. The comparability of the Virginia Key and Samoa results suggest that these ratios may be applicable over a wide area of the world ocean. Estimates from nonconcurrent data for the washout ratios at Bermuda were factors of two to four higher. Regression equations for washout ratio vs event rainfall (logW = loga + blogR) at Virginia Key were essentially the same for all three constituents with ‘a’ ranging from 1100 to 1300 and ‘b’ ranging from −0.26 to −0.29. The coefficients for American Samoa were markedly different: ‘a’ ranged from 2900 to 3600 and ‘b’ ranged from −0.51 to −0.56.     

Denuder measurements of gas and aerosol species above Arctic snow surfaces at Alert 2000

Gas and aerosol measurements were made during the Polar Sunrise Experiment 2000 at Alert, Nunavut (Canada), using two independent denuder/filter systems for sampling and subsequent analysis by ion chromatography. Twelve to forty-eight hour samples were taken during a winter (9–21 February 2000) and a spring (17 April–5 May 2000) campaign. During the spring campaign, samples were taken at two different heights above the snow surface to investigate concentration differences. Total particulate NO₃⁻ is the most abundant inorganic nitrogen compound during Arctic springtime (mean 137.4 ng m⁻³). The NO₃⁻ fluxes were calculated above the snow surface to help identify processes that control snow–atmosphere exchange of reactive nitrogen compounds. We suggest that the observed fluxes of coarse particle NO₃⁻ via snow deposition may contribute to the nitrogen inventory in the snow surface. Measurements of surface snow provide experimental data that constrain the contribution of dry deposition of coarse particle NO₃⁻ to <7%. Wet deposition in falling snow appears to be the major contributor to the nitrate input to the snow.     

Partitioning of formaldehyde between air and ice at −35°C to −5°C

The equilibrium partitioning of formaldehyde (HCHO) between air and snow was studied in a series of laboratory experiments conducted at −5°C, −15°C, and −35°C, in order to understand how partitioning of HCHO between air and polar snow varies with temperature, and thus seasonally on the ice sheet. Measured partitioning coefficients were 56, 93, and 245 mol l⁻¹ atm⁻¹ for −5°C, −15°C and −35°C, respectively, showing a similar trend as the values previously estimated from field observations. Estimates of the pseudo-first-order rate coefficient for air–snow exchange for the same three temperatures were 4.1×10⁻⁴, 1.1×10⁻⁴, and 1.1×10⁻⁵ s⁻¹, respectively. This implies a time scale for air–snow equilibration of the order of hours to days for HCHO accumulated at or near the ice–air interface on snow grains. Comparing the current laboratory partitioning coefficients with those estimated from measurements of air and freshly fallen snow in Greenland during summer demonstrates that the snow is supersaturated and should degas HCHO to the surrounding air. During this degassing, polar snow should be a significant source of HCHO to the lower troposphere.     

Vertical mixing above Summit,Greenland: Insights into seasonal and high frequency variability from the radionuclide tracers 7Be and 210Pb

The activity of the natural radionuclide tracers ⁷Be and ²¹⁰Pb has been determined in bulk aerosol samples collected over 2-day intervals for nearly five full years at Summit, Greenland. Year-round sampling was conducted in three campaigns; summer 1997 to summer 1998, summer 2000 to summer 2002, and summer 2003 to present. As in previous summer campaigns at Summit, and a year-round investigation at Dye 3, variations in the activities of the tracers on short time scales were strongly correlated despite the upper troposphere/lower stratosphere source of ⁷Be and the continental surface source of ²²²Rn (precursor of ²¹⁰Pb). This behavior is attributed to boundary layer dynamics exerting the dominant control on activities in air just above the ice sheet. Aerosols and associated species are depleted from the boundary layer above the snow when a strong inversion limits exchange with the free troposphere. Episodic weakening of the inversion allows ventilation of the boundary layer. This cycle drives simultaneous decreases and increases in the radionuclide tracers. The correlation between ⁷Be and ²¹⁰Pb on seasonal and annual bases was found to be stronger than at Dye 3, and the average activity of ⁷Be was lower at Summit despite the higher elevation (3.0 versus 2.5 km). These observations indicate that the boundary layer at Summit is more effectively isolated than at Dye 3. The activity of ⁷Be at Summit peaked in June or July all 5 years, closely following the seasonality of stratospheric injection of ⁷Be into the Arctic troposphere (based on seasonality of the ¹⁰Be/⁷Be ratio previously measured at Alert, NWT). This suggests that when the boundary layer at Summit is replenished by ventilation, it receives air reflecting the composition of the mid and upper troposphere.     

Mineral particles content in recent snow at Summit (Greenland)

The mineral insoluble fraction of snowpit samples collected at Summit is investigated, representing deposition from summer 1987 to summer 1991. We attempt to describe the particles which are observed in the series, with very large seasonal variations. Elemental, mineralogical and size distribution studies are carried out on four samples selected according to the chemical profile of the snowpit (two samples from spring and two from winter) using X-ray fluorescence spectrometry and analytical transmission electron microscopy. Results indicate a large predominance of the soil-derived particles originating from arid or semi-arid regions of the Northern Hemisphere. The mineralogy clearly indicates a high contribution for the muscovite-illite associated with a low kaolinite/chlorite ratio, together with the rather lack of smectite. This supports the hypothesis of an Asian source. Several other factors are consistent with this Asian source, like the recent climatology and the good timing between the Asian dust storms period and the peak of dust concentration in the ice. The mineralogy of the insoluble particles in the snow is similar between winter and spring, suggesting that the change of concentration between the seasons is more strongly linked to changes of atmospheric parameters than changes of the source regions.     

Comparison of surrogate surface techniques for estimation of sulfate dry deposition

The dry deposition rates of sulfate particles to artificial surfaces within and above a mature hardwood forest were measured over an annual range of synoptic weather conditions. Artificial, or ‘surrogate’, surfaces representing both rough and smooth textural types included deposition buckets, petri dishes, filter paper, Teflon configurations and polycarbonate membranes. Ambient concentrations of sulfate and sulfur dioxide were also monitored.The artificial surfaces were evaluated on the basis of the magnitude of the sulfate dry deposition rates and measurement precision. Correlations between techniques and the magnitude of the deposition velocities identified technique similarities. Ambient concentrations of the sulfur oxides and the deposition rates were not well correlated. For diverse reasons, many of the techniques were found to have limited reliability. The petri dish, bucket inside and filter plate surfaces were found to represent the most precise devices for the estimation of dry deposition to smooth, complex and rough artificial surfaces, respectively. Seasonal averages for samplers exposed at all heights were 11.2, 27.7 and 71.2μg SO₄²⁻m⁻²h⁻¹, yielding mean deposition velocities to surfaces exposed within the forest canopy of 0.03,0.11 and 0.14 cm s⁻¹ and an annual estimate of the potential dry deposition to a foliated hardwood forest of 4.0, 11.5 and 21.0 kg SO₄²⁻ha⁻¹ for the petri dish, bucket inside and filter plate surfaces, respectively. The indirect ratio between deposition rates and velocities results from varying concentrations of ambient sulfate between sampling periods. The accuracy of the filter plate data is suspect due to a significant correlation with sulfur dioxide concentrations. Sulfur concentration and deposition rate gradients indicate the forest is providing a net sink for sulfur pollutants during periods with foliage.The wide range of dry deposition rates estimated from the variety of deposition surfaces emphasizes the uncertainty of the artificial surface measurement techniques. In spite of these limitations, surrogate surfaces provide an estimate of sulfate flux rates not currently obtainable from natural surfaces.     

Deposition processes of ionic constituents to snow cover

Atmospheric deposition is an important removal process of aerosol particles and gases from the atmosphere. To elucidate the relative contributions of wet and dry processes and in-cloud and below-cloud scavenging based on deposition amounts in winter at Mt. Tateyama, central Japan, we obtained daily samples (December, 2006–March, 2007) of size-segregated aerosol particles and precipitation at Senjyugahara (SJ; 475 m a.s.l.) and vertical samples of spring snow cover at Murododaira (MR, 2450 m a.s.l., 13 km distance from SJ) on the western flank of Mt. Tateyama. The NH₄⁺ and nssSO₄^2? in aerosols were mostly found in the fine fraction (<2 μm), although Na⁺, NO₃^?, and nssCa²⁺ were mainly detected in the coarse fraction (>2 μm). Average ionic concentrations (μg g^?1) in precipitation at SJ were higher about 3.8 for Na⁺ and nssCa²⁺, 3.4 for NO₃^?, 3.7 for NH₄⁺, 2.5 for nssSO₄^2? than those at MR, whereas cumulative precipitation amounts at SJ and MR were, respectively, 84 and 175 cm of water equivalent. Wet and dry deposition amounts during the study period were estimated for sites using size-segregated aerosol data, winter averages of HNO₃, NH₃, and SO₂ concentrations, and dry deposition velocities. Particle-dry deposition comprised about 3% (Na⁺) to 11% (NH₄⁺) of the total deposition at MR. The maximum amounts of gas dry deposition were estimated, respectively, as 4, 13, and 3% of the total deposition at MR for NH₄⁺, NO₃^?, and nssSO₄^2?. The relative contributions of below-cloud scavenging (BCS) between MR and SJ were estimated as considering the wet only deposition amount at MR. Higher contributions of BCS were obtained for Na⁺ (56%) and nssCa²⁺ (45%), whereas BCSs for NH₄⁺, NO₃^?, and nssSO₄^2? were lower than 28%. Ionic constituents existing predominantly in the coarse fraction showed a large contribution of BCS.     

An assessment of sulfur deposition pathways in Asia

The acid deposition model is developed and applied to assess the sulfur deposition pathways in Asia. Simulations for four seasons are conducted: February, April, August, and October. The predicted results of summer and winter are compared to measured concentration of SO₂, sulfate, and sulfate wet deposition in Japan. Further comparison of sulfate wet deposition to observations in China is made to assess the general performance of the model. The study shows that wet deposition is more important than dry deposition. It is the predominant factor in each of these four months. It is also found that rainout process, compared to washout process, make a larger contribution to sulfate wet deposition in summer and spring than in the dry months, such as October. The total sulfur wet to dry deposition ratio is 1.6 in February, 1.2 in April, 2.9 in August, and 1.9 in October.