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1.
The second Arctic Gas and Aerosol Sampling Program (AGASP-II) was conducted across the Alaskan and Canadian Arctic in April 1986, to study the in situ aerosol, and the chemical and optical properties of Arctic haze. The NOAA WP-3D aircraft, with special instrumentation added, made six flights during AGASP-II. Measurements of wind, pressure, temperature, ozone, water vapor, condensation nuclei (CN) concentration, and aerosol scattering extinction (bsp) were used to determine the location of significant haze layers. The measurements made on the first three flights, over the Arctic Ocean north of Barrow and over the Beaufort Sea north of Barter Island, Alaska are discussed in detail in this report of the first phase of AGASP II. In the Alaskan Arctic the WP-3D detected a large and persistent region of haze between 960 and 750 mb, in a thermally stable layer, on 2, 8, and 9 April 1986. At its most dense, the haze contained CN concentrations >10,000 cm–3 and bsp of 80×10–6 m–1 suggesting active SO2 to H2SO4 gas-to-particle conversion. Calculations based upon observed SO2 concentrations and ambient relative humidities suggest that 104–105 small H2SO4 droplets could have been produced in the haze layers. High concentrations of sub-micron H2SO4 droplets were collected in haze. Ozone concentrations were 5–10 ppb higher in the haze layers than in the surrounding troposphere. Outside the regions of haze, CN concentrations ranged from 100 to 400 cm–3 and bsp values were about (20–40)×10–6 m–1. Air mass trajectories were computed to depict the air flow upwind of regions in which haze was observed. In two cases the back trajectories and ground measurements suggested the source to be in central Europe.  相似文献   

2.
Airborne measurements of the emissions from natural fires, fueled by pyrites and organic materials, at the Smoking Hills in the Northwest Territories, show that they are a regionally significant source of SO2 (0.3 kg s–1 or 104 T yr–1) and particles (0.3 kg s–1). It appears likely that the Smoking Hills are a source for some of the dense, lower-level, haze layers that occur in the North American Arctic.  相似文献   

3.
Fifty flask air samples were taken during April 1986 from a NOAA WP-3D Orion aircraft which flew missions across a broad region of the Arctic as part of the second Arctic Gas and Aerosol Sampling Program (AGASP II). The samples were subsequently analyzed for both carbon dioxide (CO2) and methane (CH4). The samples were taken in well-defined layers of Arctic haze, in the background troposphere where no haze was detected, and from near the surface to the lower stratosphere. Vertical profiles were specifically measured in the vicinity of Barrow, Alaska to enable comparisons with routine surface measurements made at the NOAA/GMCC observatory. Elevated levels of both methane and carbon dioxide were found in haze layers. For samples taken in the background troposphere we found negative vertical gradients (lower concentrations aloft) for both gases. For the entire data set (including samples collected in the haze layers) we found a strong positive correlation between the methane and carbon dioxide concentrations, with a linear regression slope of 17.5 ppb CH4/ppm CO2, a standard error of 0.6, and a correlation coefficient (r2) of 0.95. This correlation between the two gases seen in the aircraft samples was corroborated by in situ surface measurements of these gases made at the Barrow observatory during March and April 1986. We also find a similar relationship between methane and carbon dioxide measured concurrenty for a short period in the moderately polluted urban atmosphere of Boulder, Colorado. We suggest that the strong correlation between methane and carbon dioxide concentrations reflects a common source region for both, with subsequent long-range transport of the polluted air to the Arctic.  相似文献   

4.
As a component of the Canadian Arctic Haze Study, held coincident with the second Arctic Gas and Aerosol Sampling Program (AGASP II), vertical profiles of aerosol size distribution (0.17 m), light scattering parameters and cloud particle concentrations were obtained with an instrumented aircraft and ground-based lidar system during April 1986 at Alert. Northwest Territories. Average aerosol number concentrations range from about 200 cm–3 over the Arctic ice cap to about 100 cm–3 at 6 km. The aerosol size spectrum is virtually free of giant or coarse aerosol particles, and does not vary significantly with altitude. Most of the aerosol volume is concentrated in the 0.17–0.50 m size range, and the aerosol number concentration is found to be a good surrogate for the SO4 = concentration of the Arctic haze aerosol. Comparison of the aircraft and lidar data show that, when iced crystal scattering is excluded, the aerosol light scattering coefficient and the lidar backscattering coefficient are proportional to the Arctic haze aerosol concentration. Ratios of scattering to backscattering, scattering to aerosol number concentration, and backscattering to aerosol number concentration are 15.3 steradians, 1.1×10–13 m2, and 4.8×10–15 m2 sr–1, respectively. Aerosol scattering coefficients calculated from the measured size distributions using Mie scattering agree well with measured values. The calculations indicate the aerosol absorption optical depth over 6 km to range between 0.011 and 0.018. The presence of small numbers of ice crystals (10–20 crystals 1–1 measured) increased light scattering by over a factor of ten.  相似文献   

5.
Summary The extent and thickness of clouds in the Arctic Basin varied considerably in space and time in the late springs and summers of 1977–1979. While, on the average, clouds covered two thirds or more of the basin at any one time, cloud-free episodes were particularly common from the middle of June to late July and persisted locally for several days or even weeks. The central Arctic was less cloudy than the ocean zones closer to the coast in spring, but more cloudy in summer. Most clouds were semi-transparent, allowing recognition of underlying surface features. Optically thick clouds with middle and high level tops were associated with low pressure systems and with atmospheric flows from lower latitudes at the surface and aloft. Cloud-free skies were most frequent in high pressure cells. Climate models used to assess the impact of CO2 and other trace gases on the radiation budget in the high latitudes should account for the heterogeneity of cloud extent and thickness in the Arctic Basin.With 12 Figures  相似文献   

6.
Thermal and optical techniques were used at Barrow, Alaska during AGASP II (3/20/86–4/7/86) to measure in-situ variability of major aerosol components present in Arctic Haze. The experiment provided continuous data on the concentration, size distribution and relative proportions of sulfate species and refractory aerosol for particle diameters of 0.15 to 5 m. Filter samples were also taken for determination of aerosol optical absorption due to soot (EC-elemental carbon). Although pronounced haze events were absence during this period the haze aerosol present varied in concentration between 2 and 6 g/m3 but showed little change in relative constituents. Apart from local influences, the optical data indicated a persistent fine-mode sulfate aerosol with a NH4 +/SO4 – molar ratio of about 0.4 and a refractory component of somewhat less than 10% by mass. A preliminary comparison of soot estimates determined from the light absorption data with the size distributions of refractory aerosol observed independently by the optical particle counter showed good agreement during the sample period. In the absence of local pollution, values of single scatter albedo derived from light scattering and light absorption showed similar variation about the average value of 0.86 found by us during flights north of Barrow three years earlier during AGASP I.  相似文献   

7.
Thirty-six aerosol filter samples collected in tropospheric Arctic haze layers, in the stratosphere, and in the marine boundary layer during the 1983 Arctic Gas and Aerosol Sampling Program were analyzed for trace elements using instrumental neutron activation analysis. Average crustal dust concentrations were 540 ng/m3 and 330 ng/m3 for samples collected in Arctic haze over the North American and Norwegian Arctic, respectively. An average marine salt concentration of 120 ng/m3 was obtained for haze samples collected above the marine boundary layer on both sides of the Arctic.Meteorological and wind trajectory information were used to identify specific haze transport pathways, which brought relatively unmixed aerosol from the central Soviet Union into the AGASP sampling areas. Results from individual filters collected within these transport zones are discussed, with emphasis on certain trace metal ratos which have been proposed by other researchers as discriminators of aerosols from different source regions. Our aircraft-collected data are compared with previously-collected ground-based measurements, and show reasonably good agreement for most tracer elements and ratios. Specifically, we have determined the As/Sb ratio tracer, named by other researchers as the most effective elemental discriminator of aerosol from the central Soviet Union, to be approximately 5–6. This relatively high tracer value is consistent with previous ground-based findings. A significantly lower V/Sb ratio was observed throughout this study, possibly indicating a change in the source signature.  相似文献   

8.
Based on 1-year cloud measurements with radar and microwave radiometer broadband solar radiative transfer simulations were performed to quantify the impact of different ice crystal shapes of Arctic mixed-phase clouds on their radiative properties (reflectance, transmittance and absorptance). The ice crystal shape effects were investigated as a function of microphysical cloud properties (ice volume fraction fi, ice and liquid water content IWC and LWC, mean particle diameter DmI and DmW of ice/water particle number size distributions, NSDs).The required NSDs were statistically derived from radar data. The NSD was composed of a liquid and a solid mode defined by LWC, DmW (water mode) and IWC, DmI (ice mode). It was found that the ratio of DmI and DmW determines the magnitude of the shape effect. For mixed-phase clouds with DmI ≤ 27 μm a significant shape effect was obtained. The shape effect was almost insensitive with regard to the solar zenith angle, but highly sensitive to the ice volume fraction of the mixed-phase cloud. For mixed-phase clouds containing small ice crystals (DmI ≤ 27 μm) and high ice volume fractions (fi > 0.5) crystal shape is crucial. The largest shape effects were observed assuming aggregates and columns. If the IWC was conserved the shape effect reaches values up to 0.23 in cloud reflectance and transmittance. If the ice mode NSD was kept constant only a small shape effect was quantified (≤ 0.04).  相似文献   

9.
Measurements at Barrow during the second Arctic Gas and Aerosol Sampling Program (AGASP-II), conducted in April 1986, showed no rapid long-range transport from lower-latitude source regions to Barrow, and only limited vertical transport from above the boundary layer to the surface. New aerosol size distribution measurements in the 0.005–0.1 m diameter size range using a Nuclepore-filter diffusion battery apparatus showed a median diameter of about 0.01 m during times of high condensation nucleus (CN) concentrations. Aerosol black carbon concentrations exceeding 400 ng m–3 were detected at the surface and were more strongly correlated with CN concentrations than with aerosol scattering extinction (sp), suggesting that aerosol carbon was generally associated with small particles rather than large particles. Measurements at Barrow during AGASP-I, conducted in March–April 1983, showed a series of aerosol events detected at the ground that were caused by rapid long-range transport paths to the vicinity of Barrow from Eurasia. These events were strongly correlated with aerosol loading in the vertical column (optical depth).  相似文献   

10.
Cascade impactor samples were collected over the Alaskan Arctic during the first three research flights of AGASP-II. These samples were analyzed using analytical electron microscopy to determine the morphology, mineralogy and elemental composition of individual particles. For analytical considerations, a typical impactor sample was run for approximately 20 min, thus giving excellent time resolution of discrete events.Samples collected during flights 201 and 202 consisted of stratospheric aerosol and lower-altitude haze samples. Stratospheric samples were characterized by moderate loadings of H2SO4 droplets with relatively few particles of other types. Samples collected in tropospheric haze layers generally exhibited light-to-moderate particle loadings. H2SO4 was again the most prevalent species, with crustal and anthropogenic particles also observed. One sample taken over south-central Alaska near the end of flight 203 showed high concentrations of solid crustal particles, with relatively little associated H2SO4. Giant particles larger than 5 m were occasionally observed in this aerosol. The composition of this material closely matches that of bulk ash from the Mt. Augustine volcano, which erupted 9–13 days before collection of this sample. This brings forth the possibility that pockets of ash-rich aerosol existed over parts of south and central Alska during the AGASP-II field mission. There is no evidence that these volcanic aerosols were present in the AGASP study area north of the Brooks Range.  相似文献   

11.
An energy budget model is used to study the effect on Arctic climate of optically active aerosol in the Arctic atmosphere. The dependence of the change in surface temperature on the vertical distribution of the aerosol and on the radiative properties of the aerosol-free atmosphere, the Arctic surface, and the aerosol, itself, are calculated. An extensive sensitivity analysis is performed to assess the degree to which the results of the model are dependent upon the assumptions underlying it.List of Symbols Used I 0 Solar flux at the top of the Arctic Atmosphere (Arctic here means 70° N latitude to the pole) - a S Surface albedo of the Arctic (a S c is the value of surface albedo at which the sign of the surface temperature perturbation changes) - Reflection coefficient of the aerosol-free Arctic atmosphere - Absorption coefficient of the aerosol-free Arctic atmosphere - Transmission coefficient of the aerosol-free Arctic atmosphere - RI 0 Total flux of sunlight reflected from the Arctic - A A I 0 Total flux of sunlight absorbed in the Arctic atmosphere - A S I 0 Total flux of sunlight absorbed at the Arctic surface - A aer I 0 Total flux of sunlight absorbed in the Arctic aerosol - Q A Net atmospheric flow of energy, per unit of Arctic surface area, north across 70° N latitude - Q S Net oceanic flow of energy, per unit of Arctic surface area, north across 70° N latitude - E Convective plus latent heat fluxes from surface to atmosphere - F A Net flow of energy to the Arctic atmosphere - F S Net flow of energy to the Arctic surface - T A An effective temperature of the Arctic atmosphere - T S Surface temperature of the Arctic - w Single-scattering albedo of the aerosol - t Optical depth of the aerosol - g Fraction of incident radiation scattered forward by the aerosol - Reflection coefficient of the aerosol - Absorption coefficient of the aerosol - Transmission coefficient of the aerosol - p,q Number of atmospheric layers and the inverse of the fraction of incident IR absorbed in each layer in the energy budget model - F,G,H Measures of the amount of IR-active atmosphere above the surface, the aerosol, and the clouds  相似文献   

12.
During the second Arctic Gas and Aerosol Sampling Program conducted in April 1986, we performed measurements of the optically absorbing carbonaceous component of the ambient aerosol from the NOAA WP-3D aircraft operating between sea level and 10 km altitude. We collected the aerosol of filters that were exposed for several hours; we also operated the aethalometer to measure the concentration of aerosol black carbon in real time. The filter analyses represent averages over the altitude range and time span during which the filter was collecting. The real-time results were sorted by altitude to calculate vertical profiles of black carbon concentration. Values typically ranged from 300 to 500 ng m–3 at lower altitudes, decreasing gradually to 25 to 100 ng m–3 at 8–10 km. Strong stratification at lower altitudes was frequently observed. The magnitude of these concentrations suggests that the sources are distant regions of considerable fuel consumption. The presence of this material in the tropospheric column and its probable deposition to the high-albedo surface may result in perturbations of the solar radiation balance. The concentrations measured at the highest altitudes may mean that particulate carbon and accompanying emissions for which it is a tracer are mixing into the stratosphere.  相似文献   

13.
Chemical characteristics of haze during summer and winter in Guangzhou   总被引：33，自引：0，他引：33  
Airborne particles were collected with a 10-stage MOUDI and a PM10 sampler in Guangzhou, China, during both haze and normal days in the summer of 2002 and 2003, and winter 2002. The characteristics of PAHs, organic carbon, elemental carbon and water-soluble inorganic ions were studied under four periods (summer normal, summer haze, winter normal and winter haze). In this study, secondary pollutants (OC, SO42−, NO3− and NH4+) were the major chemical components and appeared to show a remarkably rapid increase from normal to haze days. The particle mass size distributions were bimodal and dominated by fine particles in haze days. A significantly higher OC/EC ratio was found in haze days (3.2–4.7) compared to normal days (1.8–2.8), indicating secondary organic aerosol formation might be significant during haze days. Correlation analysis between visibility and chemical species showed that the major scattering species were TC (total carbon) and sulfate in normal days and nitrate and TC in haze days, respectively. Simultaneously, correlation analysis between visibility and meteorological factors demonstrated that visibility increased with both temperature and wind speed, while it decreased with relative humidity. Furthermore, the relatively higher value of IcdP/(BghiP + IcdP) and the low value of Cmax, CPI, and BghiP/BeP in winter haze could be due to the growth of motor vehicle usage and energy consumption in winter.  相似文献   

14.
A model is developed to simulate the potential temperature and the height of the mixed layer under advection conditions. It includes analytic expressions for the effects of mixed-layer conditions upwind of the interface between two different surfaces on the development of the mixed layer downwind from the interface. Model performance is evaluated against tethersonde data obtained on two summer days during sea breeze flow in Vancouver, Canada. It is found that the mixed-layer height and temperature over the ocean has a small but noticeable effect on the development of the mixed layer observed 10 km inland from the coast. For these two clear days, the subsidence velocity at the inversion base capping the mixed layer is estimated to be about 30 mm s–1 from late morning to late afternoon. When the effects of subsidence are included in the model, the mixed-layer height is considerably underpredicted, while the prediction for the mean potential temperature in the mixed layer is considerably improved. Good predictions for both height and temperature can be obtained when values for the heat entrainment ratio,c, 0.44 and 0.68 for these two days respectively for the period from 1000 to 1300 LAT, were used. These values are estimated using an equation including the additional effects on heat entrainment due to the mechanical mixing caused by wind shear at the top of the mixed layer and surface friction. The contribution of wind shear to entrainment was equal to, or greater than, that from buoyant convection resulting from the surface heat flux. Strong wind shear occurred near the top of the mixed layer between the lower level inland flow and the return flow aloft in the sea breeze circulation.Symbols c entrainment parameter for sensible heat - c p specific heat of air at constant pressure, 1010 J kg–1 K–1 - d 1 the thickness of velocity shear at the mixed-layer top, m - Q H surface sensible heat flux, W m–2 - u m mean mixed-layer wind speed, m s–1 - u * friction velocity at the surface, m s–1 - w subsidence velocity, m s–1 - W subsidence warming,oC s–1 - w e entrainment velocity, m s–1 - w * convection velocity in the mixed layer, m s–1 - x downwind horizontal distance from the water-land interface, m - y dummy variable forx, m - Z height above the surface, m - Z i height of capping inversion, m - Z m mixed-layer depth, i.e.,Z i–Zs, m - Z s height of the surface layer, m - lapse rate of potential temperature aboveZ i, K m–1 - potential temperature step atZ i, K - u h velocity step change at the mixed-layer top - m mean mixed-layer potential temperature, K  相似文献   

15.
During April 1986, as part of an international arctic air chemistry study (AGASP-2), ground level observations of aerosol trace elements, oxides of sulphur and nitrogen and particle number size distribution were made at Alert Canada (82.5N, 62.3W). Pollution haze was evident as indicated by daily aerosol number (size > 0.15 m diameter) and SO4 = concentrations in the range 125 – 260 cm–3 and 1.6 – 4.5 g m–3, respectively. Haze and associated acidic gases tended to increase throughout the period. SO2 and peroxyacetylnitrate (PAN) mixing ratios were in the range 140 – 480 and 370 – 590 ppt(v), respectively. About 88% of the total end-product nitrogen was in the form of PAN. In air dried to 2% relative humidity by warming to room temperature, the aerosol mass size distribution had a major mode at 0.3 m diameter and a minor one at 2.5 m. Aerosol mass below 1.5 m was well correlated with SO4 =, K+ and PAN. There was a steady increase in the oxidized fraction of total airborne sulphur and nitrogen oxide throughout April as the sun rose above the horizon and remained above. The mean oxidation rate of SO2 between Eurasia and Alert was estimated as 0.25 – 0.5% h–1. The molar ratio of total nitrogen oxide to total sulphur oxide in the arctic atmosphere (0.67±0.17) was comparable to that in European emissions. A remarkably strong inverse correlation of filterable Br and O3 led to the conclusion that O3 destruction and filterable Br production below the Arctic surface radiation inversion is associated with tropospheric photochemical reactions involving naturally occurring gaseous bromine compounds.  相似文献   

16.
Measurements of NOx (NO +NO2) and the sum of reactive nitrogenconstituents, NOy, were made near the surface atAlert (82.5°N), Canada during March and April1998. In early March when solar insolation was absentor very low, NOx mixing ratios were frequentlynear zero. After polar sunrise when the sun was abovethe horizon for much or all of the day a diurnalvariation in NOx and NOy was observed withamplitudes as large as 30–40 pptv. The source ofactive nitrogen is attributed to release from the snowsurface by a process that is apparently sensitized bysunlight. If the source from the snowpack is a largescale feature of the Arctic then the diurnal trendsalso require a competing process for removal to thesurface. From the diurnal change in the NO/NO2ratio, mid-April mixing ratios for the sum of peroxyand halogen oxide radicals of 10 pptv werederived for periods when ozone mixing ratios were inthe normal range of 30–50 ppbv. Mid-day ozoneproduction and loss rates with the active nitrogensource were estimated to be 1–2 ppbv/day and in nearbalance. NOy mixing ratios which averaged only295±66 pptv do not support a large accumulation inthe high Arctic surface layer in the winter and springof 1998. The small abundance of NOy relative tothe elevated mixing ratios of other long-livedanthropogenic constituents requires that reactivenitrogen be removed to the surface during transport toor during residence within the high Arctic.  相似文献   

17.
During two measuring campaigns in early spring 1994 and 1995 (March/April) and one campaign in summer 1994, measurements of ozone, PAN, sulfur dioxide, nitric acid, and particulate nitrate, sulfate, and ammonium (only 1995) were recorded in the Arctic. Observations were made by aircraft at various sites in the eastern and western Arctic. Ozone concentrations showed a steady increase with altitude both in spring and summer. During five flights in springtime, low ozone events (LOEs) could be observed near the surface and up to altitudes of 2000 m. SO2 background concentrations, ranging from detection limit (0.5 nmol/m3) to 5 nmol/m3, were observed during both spring and summer. Distinct maxima up to 55 nmol/m3 in lower altitudes were only obtained in springtime. Concentrations of the organic nitrate PAN were within a similar range as those of the inorganic nitrate HNO3 during spring campaigns. In contrast, concentrations of particulate nitrate were one half an order of magnitude lower. HNO3 concentrations increased significantly with altitude. Evidently, HNO3 was intruded from the stratosphere into the troposphere. Sulfate concentrations ranged between 5 and 30 nmol/m3; ammonium concentrations were obtained within a range from 10 to 50 nmol/m3.  相似文献   

18.
Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO2), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO4 2-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10–12; 24 ppt=1 nmol m–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m–2 d–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO2 concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO2 in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO2. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO2 by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO2 and one-third to MSA. On the other hand, MSA/nss-SO4 2- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO4 2- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO2, nss-SO4 2- values decreased significantly in the middle FT. NH4 +/nss-SO4 2- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium.  相似文献   

19.
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO4 2–), sodium (Na+), ammonium (NH4 +), and nitrate (NO3 –) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m–3 (STP). The nonsea-salt sulfate (ns-SO4 2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO4 2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na+ and NO3 –, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.  相似文献   

20.
Aerosol chemical composition and trace gas measurements were made at twolocations on the northeastern peninsula of Tenerife during the ACE-2HILLCLOUD experiment, between 28 June and 23 July 1997. Measurementswere made of coarse (#gt;2.5 m aerodynamic diameter) and fine (#lt; 2.5m) aerosol Cl–, NO3 –,SO4 2–, non-sea saltSO4 2– (NSSS),CH3SO3 – (MSA) andNH4 +, and gas phase dimethylsulphide (DMS), HCl,HNO3, SO2, CH3COOH, HCOOH andNH3. Size distributions were measured using a cascadeimpactor. Results show that in marine air masses NSSS and MSA wereformed via DMS oxidation, with additional NSSS present in air massescontaining a continental component. Using a Eulerian box model approachfor aerosols transported between upwind and downwind sites, a mean NSSSproduction rate of 4.36 × 10–4 gm–3 s–1 was calculated for daytimeclear sky periods (highest insolation), with values for cloudy periodsduring daytime and nighttime of 3.55 × 10–4 and2.40 × 10–4 g m–3s–1, respectively. The corresponding rates for MSA were6.23 × 10–6, 8.49 × 10–6and 6.95 × 10–6 g m–3s–1, respectively. Molar concentration ratios forMSA/NSSS were 8.7% (1.8–18.2%) and 1.9%(1.3–3.5%) in clean and polluted air masses, respectively.Reactions occurring within clouds appeared to have a greater influenceon rates of MSA production, than of NSSS, while conversely daytime gasphase reactions were more important for NSSS. For MSA, nighttimein-cloud oxidation rates exceeded rates of daytime gas phase productionvia OH oxidation of DMS. NSSS, MSA and ammonium had trimodal sizedistributions, with modes at 0.3, 4.0 and >10.0 m (NSSS andNH4 +), and 0.3, 1.5 and 4.0 m (MSA). Nosignificant production of other aerosol species was observed, with theexception of ammonium, which was formed at variable rates dependent onneutralisation of the aerosol with ammonia released from spatiallynon-uniform surface sources. Seasalt components were mainly present incoarse particles, although sub-micrometre chloride was also measured.Losses by deposition exceeded calculated expectations for all species,and were highest for the seasalt fraction and nitrate.  相似文献   

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